FN Thomson Reuters Web of Science™ VR 1.0 PT S AU Buss, JH Smith, RP Coslovich, G Kaindl, RA AF Buss, J. H. Smith, R. P. Coslovich, G. Kaindl, R. A. BE Betz, M Elezzabi, AY Tsen, KT TI Broadband Transient THz Conductivity of the Transition-Metal Dichalcogenide MoS2 SO ULTRAFAST PHENOMENA AND NANOPHOTONICS XIX SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Ultrafast Phenomena and Nanophotonics XIX CY FEB 08-11, 2015 CL San Francisco, CA SP SPIE, FEMTOLASERS Produkt GmbH DE ultrafast dynamics; THz spectroscopy; electron-hole pairs; many-particle interactions; non-equilibrium charge transport; transition-metal dichalcogenides; molybdenum disulfide; MoS2 ID INSULATOR-TRANSITION; HETEROSTRUCTURES; TRANSISTORS; CRYSTALS AB The transient dynamics of transition-metal dichalcogenides is of significant interest for clarifying fundamental many-particle interactions at the nanoscale as well as for novel applications. We report an ultrafast terahertz study up to 7 THz of the lamellar semiconductor MoS2 to access the non-equilibrium conductivity of photo-excited indirect e-h pairs in this multi-layered parent compound. While the equilibrium transport is Drude-like, near-IR optical excitation results in a complex photo-induced conductivity that consists of two components. Mobile charge carriers dominate the low frequency response below 2 THz, while at low temperatures an additional excess conductivity is observed that is enhanced around 4 THz. Two time scales appear in the dynamics: a slow ns relaxation due to non-radiative recombination and a faster sub-100 ps decay connected to the high-frequency THz feature. We discuss the broad THz peak within a model of intra-excitonic transitions in MoS2. It agrees well with the expected binding energy and oscillator strength, yet results in an anomalous temperature dependence of the exciton fraction requiring an electronically inhomogeneous phase. C1 [Buss, J. H.; Smith, R. P.; Coslovich, G.; Kaindl, R. A.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. RP Buss, JH (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. NR 23 TC 0 Z9 0 U1 5 U2 18 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-1-62841-451-6 J9 PROC SPIE PY 2015 VL 9361 AR 93611J DI 10.1117/12.2080748 PG 7 WC Engineering, Electrical & Electronic; Optics; Physics, Applied SC Engineering; Optics; Physics GA BC6OW UT WOS:000354276800020 ER PT S AU Coslovich, G Behl, S Huber, B Bechtel, HA Sasagawa, T Martin, MC Kaindl, RA AF Coslovich, G. Behl, S. Huber, B. Bechtel, H. A. Sasagawa, T. Martin, M. C. Kaindl, R. A. BE Betz, M Elezzabi, AY Tsen, KT TI Nanoscale Charge-order Dynamics in Stripe-phase Nickelates Probed via Ultrafast THz Spectroscopy SO ULTRAFAST PHENOMENA AND NANOPHOTONICS XIX SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Ultrafast Phenomena and Nanophotonics XIX CY FEB 08-11, 2015 CL San Francisco, CA SP SPIE, FEMTOLASERS Produkt GmbH DE ultrafast dynamics; nickelate; THz spectroscopy; pseudogap; phonon dynamics; charge order; stripes ID SUPERCONDUCTIVITY; PSEUDOGAP AB We discuss equilibrium and ultrafast optical pump-THz probe spectroscopy of the model stripe-ordered system La1.75Sr0.25NiO4. We present a multi-oscillator analysis of the phonon bending mode splitting observed at low temperatures in equilibrium, along with a variational model for the transient THz reflectivity variations. The low temperature splitting is directly related to the formation of the long-range stripe-order, while the background conductivity is reminiscent of the opening of the mid-IR pseudogap. Ultrafast experiments in the multi-THz spectral range show strong THz reflectivity variations around the phonon bending mode frequency (approximate to 11 THz). C1 [Coslovich, G.; Behl, S.; Huber, B.; Kaindl, R. A.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mat Sci Div, Berkeley, CA 94720 USA. [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 2268503, Japan. RP Coslovich, G (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mat Sci Div, Berkeley, CA 94720 USA. EM GCoslovich@lbl.gov RI Sasagawa, Takao/E-6666-2014 OI Sasagawa, Takao/0000-0003-0149-6696 NR 14 TC 0 Z9 0 U1 0 U2 8 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-1-62841-451-6 J9 PROC SPIE PY 2015 VL 9361 AR 93611F DI 10.1117/12.2080724 PG 6 WC Engineering, Electrical & Electronic; Optics; Physics, Applied SC Engineering; Optics; Physics GA BC6OW UT WOS:000354276800019 ER PT J AU Moon, S Zhang, XS Gao, J Fezzaa, K Dinfresne, E Wang, J Xie, XB Wang, FK Lai, MC AF Moon, Seoksu Zhang, Xusheng Gao, Jian Fezzaa, Kamel Dinfresne, Eric Wang, Jin Xie, Xingbin Wang, Fengkun Lai, Ming-Chia TI MORPHOLOGICAL EXPLORATION OF EMERGING JET FLOWS FROM MULTI-HOLE DIESEL INJECTORS AT DIFFERENT NEEDLE LIFTS SO ATOMIZATION AND SPRAYS LA English DT Article DE multi-hole nozzle; multi-orifice injector; needle lift; liquid fuel jet; X-ray phase-contrast imaging ID VORTEX FLOW; LIQUID-JET; CAVITATION; PRESSURE; DYNAMICS AB The current study takes a morphological approach to interpret the emerging jet flows from multi-hole diesel injectors. Several types of multi-hole injectors, a six-hole injector and two two-hole injectors with different needle control mechanisms, were used to investigate the emerging jet flows and related flow breakup at different needle lifts. A short X-ray pulse with 150 ps duration was used to visualize the near-field morphologies of the emerging jet flows using an ultrafast X-ray phase-contrast imaging technique. A few X-ray pulses with 68 ns periodicity were also used to analyze the dynamics of the emerging jet flows by tracking the movement of the structures inside the spray. At first, the effects of needle lift on emerging flow pattern and breakup were investigated using a six-hole injector under practical injection conditions. A highly expanding spray was observed at the low needle lifts. The degree of flow expansion was however suppressed with an increase in the needle lift. The higher degree of flow expansion at the low needle lifts promoted the flow breakup and increased the spray deceleration rate with an increase in the axial distance. Then, a detailed morphological study of the emerging flows was performed using two-hole nozzles under low injection pressures to slow down the flow breakup in order to figure out the intrinsic nature of the emerging flows associated with the nozzle internal flow. The phase-contrast images revealed clear morphologies of several branching flows inside the spray having different flowing directions and stretching the spray three-dimensionally that originate from complex nozzle internal flow pattern. The degree of flow expansion associated with the branching flows appeared differently with the needle lift with formation of various flow structures: cone shaped, stretched thin, and cylindrical. At certain needle lifts, the branching flows sometimes formed a couple of microwavelets inside the spray having different instability frequencies, indicating different origins of each flow associated with nozzle internal flow. Increasing ambient gas density did not alter the branching characteristics of the flows significantly, while increasing injection pressure and reducing the fuel viscosity significantly altered the branching flow characteristics. C1 [Moon, Seoksu] Natl Inst Adv Ind Sci & Technol, Energy Technol Res Inst, Tsukuba, Ibaraki, Japan. [Moon, Seoksu; Zhang, Xusheng; Gao, Jian; Fezzaa, Kamel; Dinfresne, Eric; Wang, Jin] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. [Zhang, Xusheng] Shanghai Maritime Univ, Merchant Marine Coll, Shanghai, Peoples R China. [Gao, Jian] Gen Motors Global Res & Dev, Propuls Syst Res Lab, Warren, MI USA. [Xie, Xingbin; Wang, Fengkun; Lai, Ming-Chia] Wayne State Univ, Dept Mech Engn, Detroit, MI 48202 USA. RP Moon, S (reprint author), Natl Inst Adv Ind Sci & Technol, Energy Technol Res Inst, Tsukuba, Ibaraki, Japan. EM ss.moon@aist.go.jp FU U.S. Department of Energy (DOE), Office of Science/Basic Energy Science and Energy Efficiency and Renewable Energy/Vehicle Technology; Ministry of Economy, Industry, and Trade (METI) of Japan as a part of Japan-U.S. cooperation project for research and standardization of Clean Energy Technologies; DOE in the United States; METI in Japan; Deere Company FX This work and the use of the APS were supported by U.S. Department of Energy (DOE), Office of Science/Basic Energy Science and Energy Efficiency and Renewable Energy/Vehicle Technology. This work was also partially supported by the Ministry of Economy, Industry, and Trade (METI) of Japan as a part of Japan-U.S. cooperation project for research and standardization of Clean Energy Technologies. The authors thank the DOE in the United States and METI in Japan for financial support, as well as Deere & Company, and Dr. Richard Windsor of John Deere, for hardware support. NR 18 TC 7 Z9 7 U1 3 U2 6 PU BEGELL HOUSE INC PI DANBURY PA 50 NORTH ST, DANBURY, CT 06810 USA SN 1044-5110 EI 1936-2684 J9 ATOMIZATION SPRAY JI Atom. Sprays PY 2015 VL 25 IS 5 BP 375 EP 396 PG 22 WC Engineering, Multidisciplinary; Engineering, Chemical; Engineering, Mechanical; Materials Science, Multidisciplinary; Physics, Applied SC Engineering; Materials Science; Physics GA CH3LU UT WOS:000353933000002 ER PT J AU Pickett, LM Genzale, CL Manin, J AF Pickett, L. M. Genzale, C. L. Manin, J. TI UNCERTAINTY QUANTIFICATION FOR LIQUID PENETRATION OF EVAPORATING SPRAYS AT DIESEL-LIKE CONDITIONS SO ATOMIZATION AND SPRAYS LA English DT Article DE diesel sprays; evaporation; liquid length; extinction; light scatter ID ENGINE; BEHAVIOR AB Seeking to quantify the liquid volume fraction at the measured liquid penetration length for more forthright comparison to CFD results, we compared 10 different light-scatter and extinction diagnostics for measurement of the "liquid length" of an evaporating diesel spray. Results show that light-scatter imaging is sensitive to the orientation of the illumination source, producing different maximum intensity locations depending on the optical setup. However, the scattered intensity from different setups can be normalized to provide similar liquid length values if the appropriate reference intensity is known. Light-extinction diagnostics are more quantitative because of a built-in reference light intensity, but can be sensitive to beam-steering effects due to refractive index gradients. The most quantitative diagnostic in this study is a small laser beam with large collection optics to accommodate beam steering. Using a liquid length defined based on 3% of the maximum scatter intensity and the measured optical thickness at this same axial location, we estimate an expected range of liquid volume fraction at this position for the "spray A" conditions of the Engine Combustion Network. Even though there is a possibility that this condition has supercritical mixtures where distinct droplets do not exist, we apply Mie scatter theory with a range of droplet diameters (0.1-10 mu m) to mimic how light may scatter at liquid surfaces where density gradients remain sharp and light effectively scatters as if there were a gas-liquid interface. With a measured liquid path length of 1.4 mm, the upper-bound estimate for the path-length-averaged liquid volume fraction is 0.15%. C1 [Pickett, L. M.; Manin, J.] Sandia Natl Labs, Livermore, CA 94551 USA. [Genzale, C. L.] Georgia Inst Technol, Atlanta, GA 30332 USA. RP Pickett, LM (reprint author), Sandia Natl Labs, POB 969,MS9053, Livermore, CA 94551 USA. EM LMPicke@sandia.gov FU U.S. Department of Energy, Office of Vehicle Technologies; United States Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX Support for this research was provided by the U.S. Department of Energy, Office of Vehicle Technologies. The research at Sandia National Laboratories was performed at the Combustion Research Facility, Livermore, California. 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 No. DE-AC04-94AL85000. NR 32 TC 2 Z9 2 U1 2 U2 7 PU BEGELL HOUSE INC PI DANBURY PA 50 NORTH ST, DANBURY, CT 06810 USA SN 1044-5110 EI 1936-2684 J9 ATOMIZATION SPRAY JI Atom. Sprays PY 2015 VL 25 IS 5 BP 425 EP 452 PG 28 WC Engineering, Multidisciplinary; Engineering, Chemical; Engineering, Mechanical; Materials Science, Multidisciplinary; Physics, Applied SC Engineering; Materials Science; Physics GA CH3LU UT WOS:000353933000004 ER PT J AU Battistoni, M Duke, DJ Swantek, AB Tilocco, FZ Powell, CF Som, S AF Battistoni, Michele Duke, Daniel J. Swantek, Andrew B. Tilocco, F. Zak Powell, Christopher F. Som, Sibendu TI EFFECTS OF NONCONDENSABLE GAS ON CAVITATING NOZZLES SO ATOMIZATION AND SPRAYS LA English DT Article DE injector nozzle flow; cavitation; noncondensable gas; mixture model ID DIESEL INJECTOR NOZZLES; RELAXATION MODEL; FLOW; SIMULATION AB This paper focuses on the analysis of low-pressure regions inside fuel injector nozzles, where fuel vapor formation (strictly referred to as cavitation, or vaporous cavitation) and expansion of noncondensable gas (also referred to as pseudo cavitation, or gaseous cavitation) can simultaneously occur. Recently, X-ray radiography experiments of a 500 pin diameter cavitating nozzle showed that the presence of dissolved gas in the fuel can cause significant changes in the apparent distribution of projected void fraction. In this article, the effect of dissolved gas on cavitation measurements is investigated in further detail through experimentation and numerical simulations. Test conditions have been selected to have highly cavitating conditions. Tests with a standard gasoline calibration fluid and equivalent degassed fluid are compared and discussed. Numerical simulations have been conducted under the same conditions as the radiography experiments. The primary goal of the study is a quantification of the separate contributions of gas expansion as opposed to actual cavitation to the measurement of total void fraction. The multiphase flow is represented using a mixture model. Phase change is modeled via the homogeneous relaxation model. Particular attention is paid to quantifying the effective amount of noncondensable gas included in the mixture, in order to predict the response of regular and degassed fuels. The presence of dissolved gas in the multiphase flow is taken into account using a compressible fluid model with three distinct components (liquid, vapor, and gas). Issues surrounding estimation of the effective amount of noncondensable gas are discussed. Numerical simulation results match well with the experiments and indicate that when a sufficient quantity of gas is dissolved in the fuel, a void is evident in the central region of the channel that can be attributed to local expansion of noncondensed gas. Conversely, degassed fuel shows only intense cavitation at the nozzle wall, with very little contribution from noncondensed gas. C1 [Battistoni, Michele; Duke, Daniel J.; Swantek, Andrew B.; Tilocco, F. Zak; Powell, Christopher F.; Som, Sibendu] Argonne Natl Lab, Div Energy Syst, Argonne, IL 60439 USA. [Battistoni, Michele] Univ Perugia, Dept Engn, I-06100 Perugia, Italy. RP Battistoni, M (reprint author), Argonne Natl Lab, Div Energy Syst, 9700 S Cass Ave, Argonne, IL 60439 USA. EM michele.battistoni@unipg.it RI Battistoni, Michele/M-9194-2014 OI Battistoni, Michele/0000-0001-6807-9657 FU U.S. Department of Energy Office of Science laboratory [DE-AC02-06CH11357]; DOE's Office of Vehicle Technologies, Office of Energy Efficiency and Renewable Energy [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. This research was funded by DOE's Office of Vehicle Technologies, Office of Energy Efficiency and Renewable Energy under Contract No. DE-AC02-06CH11357. The authors thank Gurpreet Singh, program manager at DOE, for his support. We gratefully acknowledge the computing resources provided on "Fusion," a 3000-core computing cluster operated by the Laboratory Computing Resource Center at Argonne National Laboratory. We also acknowledge Eric Pomraning and Shaoping Quan at Convergent Science Inc. for providing support with the code and for many helpful discussions. NR 48 TC 13 Z9 13 U1 1 U2 10 PU BEGELL HOUSE INC PI DANBURY PA 50 NORTH ST, DANBURY, CT 06810 USA SN 1044-5110 EI 1936-2684 J9 ATOMIZATION SPRAY JI Atom. Sprays PY 2015 VL 25 IS 6 BP 453 EP 483 PG 31 WC Engineering, Multidisciplinary; Engineering, Chemical; Engineering, Mechanical; Materials Science, Multidisciplinary; Physics, Applied SC Engineering; Materials Science; Physics GA CH3LV UT WOS:000353933100002 ER PT J AU Ballantyne, AP Andres, R Houghton, R Stocker, BD Wanninkhof, R Anderegg, W Cooper, LA DeGrandpre, M Tans, PP Miller, JB Alden, C White, JWC AF Ballantyne, A. P. Andres, R. Houghton, R. Stocker, B. D. Wanninkhof, R. Anderegg, W. Cooper, L. A. DeGrandpre, M. Tans, P. P. Miller, J. B. Alden, C. White, J. W. C. TI Audit of the global carbon budget: estimate errors and their impact on uptake uncertainty SO BIOGEOSCIENCES LA English DT Article ID LAND-COVER CHANGE; NET PRIMARY PRODUCTION; ATMOSPHERIC CO2; INTERANNUAL VARIABILITY; SAMPLING-NETWORK; SOUTHERN-OCEAN; DIOXIDE; EMISSIONS; CYCLE; CLIMATE AB Over the last 5 decades monitoring systems have been developed to detect changes in the accumulation of carbon (C) in the atmosphere and ocean; however, our ability to detect changes in the behavior of the global C cycle is still hindered by measurement and estimate errors. Here we present a rigorous and flexible framework for assessing the temporal and spatial components of estimate errors and their impact on uncertainty in net C uptake by the biosphere. We present a novel approach for incorporating temporally correlated random error into the error structure of emission estimates. Based on this approach, we conclude that the 2 sigma uncertainties of the atmospheric growth rate have decreased from 1.2 Pg C yr(-1) in the 1960s to 0.3 Pg C yr(-1) in the 2000s due to an expansion of the atmospheric observation network. The 2 sigma uncertainties in fossil fuel emissions have increased from 0.3 Pg C yr(-1) in the 1960s to almost 1.0 Pg C yr(-1) during the 2000s due to differences in national reporting errors and differences in energy inventories. Lastly, while land use emissions have remained fairly constant, their errors still remain high and thus their global C uptake uncertainty is not trivial. Currently, the absolute errors in fossil fuel emissions rival the total emissions from land use, highlighting the extent to which fossil fuels dominate the global C budget. Because errors in the atmospheric growth rate have decreased faster than errors in total emissions have increased, a similar to 20% reduction in the overall uncertainty of net C global uptake has occurred. Given all the major sources of error in the global C budget that we could identify, we are 93% confident that terrestrial C uptake has increased and 97% confident that ocean C uptake has increased over the last 5 decades. Thus, it is clear that arguably one of the most vital ecosystem services currently provided by the biosphere is the continued removal of approximately half of atmospheric CO2 emissions from the atmosphere, although there are certain environmental costs associated with this service, such as the acidification of ocean waters. C1 [Ballantyne, A. P.; Cooper, L. A.; DeGrandpre, M.] Univ Montana, Missoula, MT 59812 USA. [Andres, R.] Oak Ridge Natl Lab, Carbon Dioxide Informat Anal Ctr, Oak Ridge, TN USA. [Houghton, R.] Woods Hole Res Ctr, Falmouth, MA USA. [Stocker, B. D.] Univ London Imperial Coll Sci Technol & Med, London, England. [Wanninkhof, R.] NOAA, Atlantic Oceanog & Meteorol Lab, Miami, FL 33149 USA. [Anderegg, W.] Princeton Univ, Princeton Environm Inst, Princeton, NJ 08544 USA. [Tans, P. P.; Miller, J. B.] NOAA, Earth Syst Res Lab, Boulder, CO USA. [Alden, C.] Stanford Univ, Palo Alto, CA 94304 USA. [White, J. W. C.] Univ Colorado, Boulder, CO 80309 USA. RP Ballantyne, AP (reprint author), Univ Montana, Missoula, MT 59812 USA. EM ashley.ballantyne@umontana.edu RI White, James/A-7845-2009; Stocker, Benjamin/K-3194-2015; OI White, James/0000-0001-6041-4684; Stocker, Benjamin/0000-0003-2697-9096; ALDEN, CAROLINE/0000-0002-5249-7800; ANDRES, ROBERT/0000-0001-8781-4979 FU NSF; NRC FX This research was supported by grants from NSF and NRC to A. P. Ballantyne. This work would not have been possible without the continuous atmospheric sampling efforts of dozens of volunteer scientists from around the world and careful measurements by researchers at NOAA ESRL. We would also like to thank Gregg Marland, Glen Peters, and one anonymous reviewer, as well as students in the Emerging Topics in Ecosystem Science seminar at the University of Montana for helpful feedback. NR 69 TC 12 Z9 12 U1 7 U2 37 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1726-4170 EI 1726-4189 J9 BIOGEOSCIENCES JI Biogeosciences PY 2015 VL 12 IS 8 BP 2565 EP 2584 DI 10.5194/bg-12-2565-2015 PG 20 WC Ecology; Geosciences, Multidisciplinary SC Environmental Sciences & Ecology; Geology GA CH2FG UT WOS:000353840500019 ER PT S AU Baba, JS Koju, V John, D AF Baba, J. S. Koju, V. John, D. BE Wax, A Backman, V TI Monte Carlo based investigation of Berry phase for depth resolved characterization of biomedical scattering samples SO BIOMEDICAL APPLICATIONS OF LIGHT SCATTERING IX SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Biomedical Applications of Light Scattering IX CY FEB 07-08, 2015 CL San Francisco, CA SP SPIE DE Berry phase; geometric phase; polarization sensitive Monte Carlo; depth resolved imaging of scattering samples; modeling anisotropic scatter; optical imaging; Polarimetry; backscattered Mueller matrix ID BACKSCATTERED POLARIZATION PATTERNS; ANGULAR-MOMENTUM; LIGHT TRANSPORT; MUELLER MATRIX; MEDIA; PROGRAMS AB The propagation of light in turbid media is an active area of research with relevance to numerous investigational fields, e.g., biomedical diagnostics and therapeutics. The statistical random-walk nature of photon propagation through turbid media is ideal for computational based modeling and simulation. Ready access to super computing resources provide a means for attaining brute force solutions to stochastic light-matter interactions entailing scattering by facilitating timely propagation of sufficient (>10(7)) photons while tracking characteristic parameters based on the incorporated physics of the problem. One such model that works well for isotropic but fails for anisotropic scatter, which is the case for many biomedical sample scattering problems, is the diffusion approximation. In this report, we address this by utilizing Berry phase (BP) evolution as a means for capturing anisotropic scattering characteristics of samples in the preceding depth where the diffusion approximation fails. We extend the polarization sensitive Monte Carlo method of Ramella-Roman, et al., 1 to include the computationally intensive tracking of photon trajectory in addition to polarization state at every scattering event. To speed-up the computations, which entail the appropriate rotations of reference frames, the code was parallelized using OpenMP. The results presented reveal that BP is strongly correlated to the photon penetration depth, thus potentiating the possibility of polarimetric depth resolved characterization of highly scattering samples, e.g., biological tissues. C1 [Baba, J. S.] Oak Ridge Natl Lab, Elect & Elect Syst Res Div, Oak Ridge, TN 37831 USA. [Baba, J. S.] Univ Tennessee, Inst Biomed Engn iBME, Knoxville, TN 37996 USA. [Koju, V.; John, D.] Univ Tennessee, Joint Inst Computat Sci, Knoxville, TN 37996 USA. [Koju, V.; John, D.] Univ Tennessee, Oak Ridge Natl Lab, Natl Inst Computat Sci, Oak Ridge, TN 37831 USA. [Koju, V.; John, D.] Middle Tennessee State Univ, Coll Basic & Appl Sci, Computat Sci Program, Murfreesboro, TN 37132 USA. RP Baba, JS (reprint author), Oak Ridge Natl Lab, Elect & Elect Syst Res Div, 1 Bethel Valley Rd,POB 2008,MS 6006, Oak Ridge, TN 37831 USA. EM babajs@ornl.gov RI Backman, Vadim/B-6689-2009 NR 15 TC 1 Z9 1 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 978-1-62841-423-3 J9 PROC SPIE PY 2015 VL 9333 AR 93330O DI 10.1117/12.2083421 PG 7 WC Engineering, Biomedical; Optics SC Engineering; Optics GA BC6FC UT WOS:000353889300006 ER PT J AU Zhang, TY Yang, MJ Benson, EE Li, ZJ van de Lagemaat, J Luther, JM Yan, YF Zhu, K Zhao, YX AF Zhang, Taiyang Yang, Mengjin Benson, Eric E. Li, Zijian van de Lagemaat, Jao Luther, Joseph M. Yan, Yanfa Zhu, Kai Zhao, Yixin TI A facile solvothermal growth of single crystal mixed halide perovskite CH3NH3Pb(Br1-xClx)(3) SO CHEMICAL COMMUNICATIONS LA English DT Article ID SENSITIZED SOLAR-CELLS; SEQUENTIAL DEPOSITION; LEAD HALIDES; EFFICIENT; TEMPERATURE AB We demonstrate a facile synthetic approach for preparing mixed halide perovskite CH3NH3Pb(Br1-xClx)(3) single crystals by the solvothermal growth of stoichiometric PbBr2 and [(1 - y)CH3NH3Br + yCH(3)NH(3)Cl] DMF precursor solutions. The band gap of CH3NH3Pb(Br1-xClx)(3) single crystals increased and the unit cell dimensions decreased with an increase in Cl content x, consistent with previous theoretical predictions. Interestingly, the Cl/Br ratio in the CH3NH3Pb(Br1-xClx)(3) single crystals is larger than that of the precursor solution, suggesting an unusual crystal growth mechanism. C1 [Zhang, Taiyang; Zhao, Yixin] Shanghai Jiao Tong Univ, Sch Environm Sci & Engn, Shanghai 200240, Peoples R China. [Yang, Mengjin; Benson, Eric E.; van de Lagemaat, Jao; Luther, Joseph M.; Zhu, Kai] Natl Renewable Energy Lab, Chem & Nanosci Ctr, Golden, CO 80401 USA. [Li, Zijian] Shanghai Jiao Tong Univ, Sch Chem & Chem Engn, Shanghai 200240, Peoples R China. [Yan, Yanfa] Univ Toledo, Dept Phys & Astron, Toledo, OH 43606 USA. [Yan, Yanfa] Univ Toledo, Ctr Photovolta Innovat & Commercializat, Toledo, OH 43606 USA. RP Zhu, K (reprint author), Natl Renewable Energy Lab, Chem & Nanosci Ctr, 15013 Denver West Pkwy, Golden, CO 80401 USA. EM Kai.Zhu@nrel.gov; yixin.zhao@sjtu.edu.cn RI Zhao, Yixin/D-2949-2012; van de Lagemaat, Jao/J-9431-2012; Zhang, Taiyang/C-7682-2017 OI Zhang, Taiyang/0000-0003-4012-2785 FU NSFC [51372151, 21303103]; U.S. Department of Energy (DOE) [DE-FOA-0000990, DE-AC36-08-GO28308] FX TZ and YZ are thankful for the support from the NSFC (Grant 51372151 and 21303103). MY, JML, and KZ acknowledge the support by the U.S. Department of Energy (DOE) SunShot Initiative under the Next Generation Photovoltaics 3 program (DE-FOA-0000990). EEB and JvdL acknowledge the support on the single crystal diffraction data analysis by the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences (DOE). The work at the National Renewable Energy Laboratory is supported by the U.S. Department of Energy under Contract No. DE-AC36-08-GO28308. NR 31 TC 33 Z9 33 U1 18 U2 117 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1359-7345 EI 1364-548X J9 CHEM COMMUN JI Chem. Commun. PY 2015 VL 51 IS 37 BP 7820 EP 7823 DI 10.1039/c5cc01835h PG 4 WC Chemistry, Multidisciplinary SC Chemistry GA CG9MI UT WOS:000353639300010 PM 25853846 ER PT J AU Darmon, JM Kumar, N Hulley, EB Weiss, CJ Raugei, S Bullock, RM Helm, ML AF Darmon, Jonathan M. Kumar, Neeraj Hulley, Elliott B. Weiss, Charles J. Raugei, Simone Bullock, R. Morris Helm, Monte L. TI Increasing the rate of hydrogen oxidation without increasing the overpotential: a bio-inspired iron molecular electrocatalyst with an outer coordination sphere proton relay SO CHEMICAL SCIENCE LA English DT Article ID ACTIVE-SITE; ENERGY; ACETONITRILE; COMPLEXES; CATALYSTS; H-2; ELECTRON; ELEMENTS; SOLVENT; MODEL AB Oxidation of hydrogen (H-2) to protons and electrons for energy production in fuel cells is currently catalyzed by platinum, but its low abundance and high cost present drawbacks to widespread adoption. Precisely controlled proton removal from the active site is critical in hydrogenase enzymes in nature that catalyze H-2 oxidation using earth-abundant metals (iron and nickel). Here we report a synthetic iron complex, (Cp-C5F4N) Fe((PNPEt)-N-Et-P-(CH2)3NMe2)(Cl), that serves as a precatalyst for the oxidation of H-2, with turnover frequencies of 290 s(-1) in fluorobenzene, under 1 atm of H-2 using 1,4- diazabicyclo [2.2.2] octane (DABCO) as the exogenous base. The inclusion of a properly tuned outer coordination sphere proton relay results in a cooperative effect between the primary, secondary and outer coordination spheres for moving protons, increasing the rate of H-2 oxidation without increasing the overpotential when compared with the analogous complex featuring a single pendant base. This finding emphasizes the key role of pendant amines in mimicking the functionality of the proton pathway in the hydrogenase enzymes. C1 [Darmon, Jonathan M.; Kumar, Neeraj; Hulley, Elliott B.; Weiss, Charles J.; Raugei, Simone; Bullock, R. Morris; Helm, Monte L.] Pacific NW Natl Lab, Ctr Mol Electrocatalysis, Div Phys Sci, Richland, WA 99352 USA. RP Helm, ML (reprint author), Pacific NW Natl Lab, Ctr Mol Electrocatalysis, Div Phys Sci, POB 999,K2-57, Richland, WA 99352 USA. EM monte.helm@pnnl.gov RI Kumar, Neeraj/M-3279-2015; Bullock, R. Morris/L-6802-2016; OI Kumar, Neeraj/0000-0001-6713-2129; Bullock, R. Morris/0000-0001-6306-4851; Helm, Monte/0000-0003-4728-8833 FU Center for Molecular Electrocatalysis, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences FX This research was supported as part of the Center for Molecular Electrocatalysis, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences. Pacific Northwest National Laboratory is operated by Battelle for the U.S. Department of Energy. NR 45 TC 14 Z9 14 U1 6 U2 28 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2041-6520 EI 2041-6539 J9 CHEM SCI JI Chem. Sci. PY 2015 VL 6 IS 5 BP 2737 EP 2745 DI 10.1039/c5sc00398a PG 9 WC Chemistry, Multidisciplinary SC Chemistry GA CG4AT UT WOS:000353223100007 ER PT J AU Hill, CH Viuff, AH Spratley, SJ Salamone, S Christensen, SH Read, RJ Moriarty, NW Jensen, HH Deane, JE AF Hill, Chris H. Viuff, Agnete H. Spratley, Samantha J. Salamone, Stephane Christensen, Stig H. Read, Randy J. Moriarty, Nigel W. Jensen, Henrik H. Deane, Janet E. TI Azasugar inhibitors as pharmacological chaperones for Krabbe disease SO CHEMICAL SCIENCE LA English DT Article ID GLOBOID-CELL LEUKODYSTROPHY; ENZYME REPLACEMENT THERAPY; LYSOSOMAL STORAGE DISEASES; ACID BETA-GLUCOSIDASE; GALC GENE; GAUCHER-DISEASE; MOLECULAR HETEROGENEITY; ALPHA-GALACTOSIDASE; JAPANESE PATIENTS; IN-VIVO AB Krabbe disease is a devastating neurodegenerative disorder characterized by rapid demyelination of nerve fibers. This disease is caused by defects in the lysosomal enzyme beta-galactocerebrosidase (GALC), which hydrolyzes the terminal galactose from glycosphingolipids. These lipids are essential components of eukaryotic cell membranes: substrates of GALC include galactocerebroside, the primary lipid component of myelin, and psychosine, a cytotoxic metabolite. Mutations of GALC that cause misfolding of the protein may be responsive to pharmacological chaperone therapy (PCT), whereby small molecules are used to stabilize these mutant proteins, thus correcting trafficking defects and increasing residual catabolic activity in cells. Here we describe a new approach for the synthesis of galacto-configured azasugars and the characterization of their interaction with GALC using biophysical, biochemical and crystallographic methods. We identify that the global stabilization of GALC conferred by azasugar derivatives, measured by fluorescence-based thermal shift assays, is directly related to their binding affinity, measured by enzyme inhibition. X-ray crystal structures of these molecules bound in the GALC active site reveal which residues participate in stabilizing interactions, show how potency is achieved and illustrate the penalties of aza/iminosugar ring distortion. The structure-activity relationships described here identify the key physical properties required of pharmacological chaperones for Krabbe disease and highlight the potential of azasugars as stabilizing agents for future enzyme replacement therapies. This work lays the foundation for new drug-based treatments of Krabbe disease. C1 [Hill, Chris H.; Spratley, Samantha J.; Read, Randy J.; Deane, Janet E.] Univ Cambridge, Cambridge Inst Med Res, Dept Haematol, Cambridge CB2 0XY, England. [Viuff, Agnete H.; Salamone, Stephane; Christensen, Stig H.; Jensen, Henrik H.] Aarhus Univ, Dept Chem, DK-8000 Aarhus C, Denmark. [Moriarty, Nigel W.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 USA. RP Jensen, HH (reprint author), Aarhus Univ, Dept Chem, Langelandsgade 140, DK-8000 Aarhus C, Denmark. EM hhj@chem.au.dk RI Read, Randy/L-1418-2013; OI Read, Randy/0000-0001-8273-0047; Deane, Janet/0000-0002-4863-0330 FU Wellcome Trust; MRC; Royal Society [UF100371]; Wellcome Trust Principal Research Fellowship [082961/Z/07/Z]; Lundbeck Foundation; Wellcome Trust Strategic Award [100140] FX We thank Stephen Graham for helpful discussions. We acknowledge Diamond Light Source for time on beamline I04-1 and I02 under proposal MX8547. C.H.H. is funded by a Wellcome Trust PhD studentship; S.J.S. is funded by an MRC PhD studentship; and J.E.D. is supported by a Royal Society University Research Fellowship (UF100371). R.J.R. is funded by a Wellcome Trust Principal Research Fellowship (Grant 082961/Z/07/Z). We are also grateful for funding from The Lundbeck Foundation to A.H.V, S.S. and H. H. J. The Cambridge Institute for Medical Research is supported by Wellcome Trust Strategic Award 100140. NR 85 TC 12 Z9 12 U1 2 U2 27 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2041-6520 EI 2041-6539 J9 CHEM SCI JI Chem. Sci. PY 2015 VL 6 IS 5 BP 3075 EP 3086 DI 10.1039/c5sc00754b PG 12 WC Chemistry, Multidisciplinary SC Chemistry GA CG4AT UT WOS:000353223100051 PM 26029356 ER PT J AU He, B Dai, J Zherebetskyy, D Chen, TL Zhang, BA Teat, SJ Zhang, QC Wang, LW Liu, Y AF He, Bo Dai, Jing Zherebetskyy, Danylo Chen, Teresa L. Zhang, Benjamin A. Teat, Simon J. Zhang, Qichun Wang, Linwang Liu, Yi TI A divergent route to core- and peripherally functionalized diazacoronenes that act as colorimetric and fluorescence proton sensors SO CHEMICAL SCIENCE LA English DT Article ID POLYCYCLIC AROMATIC-HYDROCARBONS; DISCOTIC LIQUID-CRYSTALS; PI-CONJUGATED SYSTEMS; ORGANIC SEMICONDUCTORS; PHOTOVOLTAIC DEVICES; SELF-ORGANIZATION; SOLAR-CELLS; ELECTRONICS; PLANAR; FAMILY AB Combining core annulation and peripheral group modification, we have demonstrated a divergent synthesis of a family of highly functionalized coronene derivatives from a readily accessible dichlorodiazaperylene intermediate. Various reactions, such as aromatic nucleophilic substitution, Kumada coupling and Suzuki coupling proceed effectively on alpha-positions of the pyridine sites, giving rise to alkoxy, thioalkyl, alkyl or aryl substituted polycyclic aromatic hydrocarbons. In addition to peripheral group modulation, the aromatic core structures can be altered by annulation with thiophene or benzene ring systems. Corresponding single crystal X-ray diffraction and optical studies indicate that the heteroatom linkages not only impact the solid state packing, but also significantly influence the optoelectronic properties. Moreover, these azacoronene derivatives display significant acid-induced spectroscopic changes, suggesting their great potential as colorimetric and fluorescence proton sensors. C1 [He, Bo; Chen, Teresa L.; Zhang, Benjamin A.; Liu, Yi] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA. [Dai, Jing] Zhejiang Univ, Dept Chem, Hangzhou 310027, Zhejiang, Peoples R China. [Zherebetskyy, Danylo; Wang, Linwang] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. [Teat, Simon J.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. [Zhang, Qichun] Nanyang Technol Univ, Sch Mat Sci & Engn, Singapore 639798, Singapore. RP Liu, Y (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA. EM yliu@lbl.gov RI zhang, qichun/A-2253-2011; Liu, yi/A-3384-2008; He, Bo/B-7478-2015; Zhang, Benjamin/P-7571-2015; Foundry, Molecular/G-9968-2014 OI Liu, yi/0000-0002-3954-6102; He, Bo/0000-0003-1444-4625; Zhang, Benjamin/0000-0001-8840-367X; FU Self-Assembly of Organic/Inorganic Nanocomposite Materials program; Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231] FX This work was supported by Self-Assembly of Organic/Inorganic Nanocomposite Materials program (B. H., D. Z., L.-W. W., and Y. L.), and was performed at the Molecular Foundry, with the X-ray experiment conducted at the Advanced Light Source (ALS), Lawrence Berkeley National Laboratory, all supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract no. DE-AC02-05CH11231. NR 54 TC 19 Z9 19 U1 4 U2 27 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2041-6520 EI 2041-6539 J9 CHEM SCI JI Chem. Sci. PY 2015 VL 6 IS 5 BP 3180 EP 3186 DI 10.1039/c5sc00304k PG 7 WC Chemistry, Multidisciplinary SC Chemistry GA CG4AT UT WOS:000353223100063 ER PT J AU Liu, H Zhang, CM Su, ZY Wang, K Deng, K AF Liu, Hui Zhang, Cai-Ming Su, Zhi-Yuan Wang, Kai Deng, Kai TI Research on a Pulmonary Nodule Segmentation Method Combining Fast Self-Adaptive FCM and Classification SO COMPUTATIONAL AND MATHEMATICAL METHODS IN MEDICINE LA English DT Article ID C-MEANS ALGORITHM; IMAGE SEGMENTATION; LUNG NODULES; INFORMATION AB The key problem of computer-aided diagnosis (CAD) of lung cancer is to segment pathologically changed tissues fast and accurately. As pulmonary nodules are potential manifestation of lung cancer, we propose a fast and self-adaptive pulmonary nodules segmentation method based on a combination of FCM clustering and classification learning. The enhanced spatial function considers contributions to fuzzy membership from both the grayscale similarity between central pixels and single neighboring pixels and the spatial similarity between central pixels and neighborhood and improves effectively the convergence rate and self-adaptivity of the algorithm. Experimental results show that the proposed method can achieve more accurate segmentation of vascular adhesion, pleural adhesion, and ground glass opacity (GGO) pulmonary nodules than other typical algorithms. C1 [Liu, Hui; Zhang, Cai-Ming; Su, Zhi-Yuan] Shandong Univ Finance & Econ, Sch Comp Sci & Technol, Jinan 250014, Peoples R China. [Liu, Hui; Zhang, Cai-Ming; Su, Zhi-Yuan] Digital Media Technol Key Lab Shandong Prov, Jinan 250014, Peoples R China. [Wang, Kai] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Deng, Kai] Shandong Prov Qianfoshan Hosp, Resp Dept, Jinan 250014, Peoples R China. RP Liu, H (reprint author), Shandong Univ Finance & Econ, Sch Comp Sci & Technol, Jinan 250014, Peoples R China. EM liuh_lh@126.com NR 23 TC 1 Z9 1 U1 4 U2 9 PU HINDAWI PUBLISHING CORP PI NEW YORK PA 410 PARK AVENUE, 15TH FLOOR, #287 PMB, NEW YORK, NY 10022 USA SN 1748-670X EI 1748-6718 J9 COMPUT MATH METHOD M JI Comput. Math. Method Med. PY 2015 AR 185726 DI 10.1155/2015/185726 PG 14 WC Mathematical & Computational Biology SC Mathematical & Computational Biology GA CH1KK UT WOS:000353780100001 ER PT J AU Wu, H Tang, WS Zhou, W Stavila, V Rush, JJ Udovic, TJ AF Wu, Hui Tang, Wan Si Zhou, Wei Stavila, Vitalie Rush, John J. Udovic, Terrence J. TI The structure of monoclinic Na2B10H10: a combined diffraction, spectroscopy, and theoretical approach SO CRYSTENGCOMM LA English DT Article ID SODIUM; NA; SCATTERING; NA2B12H12; BATTERIES; CRYSTAL; NUCLEAR; RB AB Neutron powder diffraction measurements of a specially synthesized (Na2B10D10)-B-11 compound, buttressed by comparative measurements and calculations of vibrational dynamics, have led to an improved, Rietveld-refined, structural model for its low-temperature monoclinic phase. The detailed atomic arrangements and phases for this compound are important for an understanding of its potential roles for fast-ion-battery and hydrogen-storage applications. A comparison of the calculated phonon densities of states (PDOSs) based on density functional theory for both the previously published structure and our new modified structure show that the PDOS of the latter is in noticeably better agreement with that experimentally observed by neutron vibrational spectroscopy. Moreover, this improved structure is predicted to have a higher stability and exhibits more reasonable separations between all neighboring sodium cations and decahydro-closo-decaborate anions. These results demonstrate the effectiveness of combining first-principles computational methods and neutron-based structural and spectroscopic techniques for determining crystal structures for such complex hydrogenous materials. C1 [Wu, Hui; Tang, Wan Si; Zhou, Wei; Rush, John J.; Udovic, Terrence J.] Natl Inst Stand & Technol, Ctr Neutron Res, Gaithersburg, MD 20899 USA. [Wu, Hui; Tang, Wan Si; Zhou, Wei; Rush, John J.] Univ Maryland, Dept Mat Sci & Engn, College Pk, MD 20742 USA. [Stavila, Vitalie] Sandia Natl Labs, Energy Nanomat, Livermore, CA 94551 USA. RP Wu, H (reprint author), Natl Inst Stand & Technol, Ctr Neutron Res, Gaithersburg, MD 20899 USA. EM hui.wu@nist.gov; udovic@nist.gov RI Wu, Hui/C-6505-2008; Zhou, Wei/C-6504-2008 OI Wu, Hui/0000-0003-0296-5204; Zhou, Wei/0000-0002-5461-3617 FU US Department of Energy (DOE) Office of Energy Efficiency and Renewable Energy [DE-EE0002978]; US DOE [DE-AC02-06CH11357] FX This work was partially supported by the US Department of Energy (DOE) Office of Energy Efficiency and Renewable Energy under grant no. DE-EE0002978. 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. The authors thank Drs. M. R. Hudson and C. M. Brown for their assistance in providing the synchrotron XRPD measurements. NR 20 TC 8 Z9 8 U1 3 U2 12 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1466-8033 J9 CRYSTENGCOMM JI Crystengcomm PY 2015 VL 17 IS 18 BP 3533 EP 3540 DI 10.1039/c5ce00369e PG 8 WC Chemistry, Multidisciplinary; Crystallography SC Chemistry; Crystallography GA CG9MW UT WOS:000353640900018 ER PT S AU Efimov, A AF Efimov, Anatoly BE Hemmati, H Boroson, DM TI Scintillations of a partially coherent beam in a laboratory turbulence: experiment and comparison to theory SO FREE-SPACE LASER COMMUNICATION AND ATMOSPHERIC PROPAGATION XXVII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Free-Space Laser Communication and Atmospheric Propagation XXVII CY FEB 08-09, 2015 CL San Francisco, CA SP SPIE DE Scintillations; Atmospheric turbulence; Free-Space Optical Communication; Partially coherent beam; Multimode fiber ID ATMOSPHERIC-TURBULENCE; PROPAGATION AB A partially coherent beam generated by coupling the output of a superluminescent diode to a multimode optical fiber is propagated through a stationary laboratory turbulence. Statistical quantities are measured as a function of propagation distance and coherence radius of the beam and are compared to existing theories in the regime of weak fluctuations. C1 Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Efimov, A (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM efimov@lanl.gov OI Efimov, Anatoly/0000-0002-5559-4147 NR 19 TC 0 Z9 0 U1 2 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 978-1-62841-444-8 J9 PROC SPIE PY 2015 VL 9354 AR 935404 DI 10.1117/12.2079473 PG 6 WC Engineering, Electrical & Electronic; Optics; Physics, Applied SC Engineering; Optics; Physics GA BC6AR UT WOS:000353710100002 ER PT S AU Lamoureux, L Adams, P Banisadr, A Stromberg, Z Graves, S Montano, G Moxley, R Mukundan, H AF Lamoureux, Loreen Adams, Peter Banisadr, Afsheen Stromberg, Zachary Graves, Steven Montano, Gabriel Moxley, Rodney Mukundan, Harshini BE Miller, BL Fauchet, PM Cunningham, BT TI An optical biosensor for detection of pathogen biomarkers from Shiga toxin-producing Escherichia coli in ground beef samples SO FRONTIERS IN BIOLOGICAL DETECTION: FROM NANOSENSORS TO SYSTEMS VII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Frontiers in Biological Detection - From Nanosensors to Systems VII CY FEB 07, 2015 CL San Francisco, CA SP SPIE DE Shiga toxin-producing Escherichia coli (STEC); lipopolysaccharides (LPS); planar optical waveguide biosensor; membrane insertion assays; amphiphilic pathogen biomarkers ID FOODBORNE ILLNESS AB Shiga toxin-producing Escherichia coli (STEC) poses a serious threat to human health through the consumption of contaminated food products, particularly beef and produce. Early detection in the food chain, and discrimination from other non-pathogenic Escherichia coli (E. coli), is critical to preventing human outbreaks, and meeting current agricultural screening standards. These pathogens often present in low concentrations in contaminated samples, making discriminatory detection difficult without the use of costly, time-consuming methods (e.g. culture). Using multiple signal transduction schemes (including novel optical methods designed for amphiphiles), specific recognition antibodies, and a waveguide-based optical biosensor developed at Los Alamos National Laboratory, we have developed ultrasensitive detection methods for lipopolysaccharides (LPS), and protein biomarkers (Shiga toxin) of STEC in complex samples (e.g. beef lysates). Waveguides functionalized with phospholipid bilayers were used to pull down amphiphilic LPS, using methods (membrane insertion) developed by our team. The assay format exploits the amphiphilic biochemistry of lipoglycans, and allows for rapid, sensitive detection with a single fluorescent reporter. We have used a combination of biophysical methods (atomic force and fluorescence microscopy) to characterize the interaction of amphiphiles with lipid bilayers, to efficiently design these assays. Sandwich immunoassays were used for detection of protein toxins. Biomarkers were spiked into homogenated ground beef samples to determine performance and limit of detection. Future work will focus on the development of discriminatory antibodies for STEC serotypes, and using quantum dots as the fluorescence reporter to enable multiplex screening of biomarkers. C1 [Lamoureux, Loreen; Graves, Steven] Univ New Mexico, Ctr Biomed Engn, Albuquerque, NM 87131 USA. [Lamoureux, Loreen; Banisadr, Afsheen; Mukundan, Harshini] Los Alamos Natl Lab, Phys Chem & Appl Spect, Los Alamos, NM 87545 USA. [Adams, Peter; Stromberg, Zachary; Montano, Gabriel] Los Alamos Natl Lab, Ctr Integrated Nanotechnol, Los Alamos, NM 87545 USA. [Lamoureux, Loreen; Mukundan, Harshini] New Mexico Consortium, Los Alamos, NM USA. [Moxley, Rodney] Univ Nebraska, Sch Vet Med & Biomed Sci, Lincoln, NE 68583 USA. RP Lamoureux, L (reprint author), Univ New Mexico, Ctr Biomed Engn, Albuquerque, NM 87131 USA. OI Adams, Peter/0000-0002-3940-8770; Moxley, Rodney/0000-0002-5377-7716; Stromberg, Loreen/0000-0003-1715-1211 NR 16 TC 1 Z9 1 U1 0 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 978-1-62841-400-4 J9 PROC SPIE PY 2015 VL 9310 AR 931004 DI 10.1117/12.2079658 PG 8 WC Nanoscience & Nanotechnology; Optics; Radiology, Nuclear Medicine & Medical Imaging SC Science & Technology - Other Topics; Optics; Radiology, Nuclear Medicine & Medical Imaging GA BC5XS UT WOS:000353630600002 ER PT J AU Sherrard, RM Carriker, NE Greeley, MS AF Sherrard, Rick M. Carriker, Neil E. Greeley, Mark S., Jr. TI How Toxic Is Coal Ash? A Laboratory Toxicity Case Study SO INTEGRATED ENVIRONMENTAL ASSESSMENT AND MANAGEMENT LA English DT Article DE Coal combustion residuals; Kingston ash spill; Toxicity testing ID AMPHIPOD HYALELLA-AZTECA; FLY-ASH; TIME BOMB; FATHEAD MINNOW; SELENIUM; FISH; POPULATIONS; EFFLUENTS; SEDIMENT; RECOVERY AB Under a consent agreement among the Environmental Protection Agency (EPA) and proponents both for and against stricter regulation, EPA is to issue a new coal ash disposal rule by the end of 2014. Laboratory toxicity investigations often yield conservative estimates of toxicity because many standard test species are more sensitive than resident species, thus could provide information useful to the rule-making. However, few laboratory studies of coal ash toxicity are available; most studies reported in the literature are based solely on field investigations. This brief communication describes a broad range of toxicity studies conducted for the Tennessee Valley Authority (TVA) Kingston ash spill, results of which help provide additional perspective on the toxicity of coal ash. Integr Environ Assess Manag 2015;11:5-9. (c) 2014 SETAC C1 [Sherrard, Rick M.] Tennessee Valley Author, Chattanooga, TN 37402 USA. [Carriker, Neil E.] Kingston Ash Recovery Project, Harriman, TN USA. [Greeley, Mark S., Jr.] Oak Ridge Natl Lab, Div Environm Sci, Oak Ridge, TN 37831 USA. RP Sherrard, RM (reprint author), Tennessee Valley Author, Chattanooga, TN 37402 USA. EM rmsherrard@tva.gov RI Greeley, Mark/D-2330-2016 OI Greeley, Mark/0000-0002-6088-5942 NR 37 TC 3 Z9 3 U1 6 U2 20 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 1551-3777 EI 1551-3793 J9 INTEGR ENVIRON ASSES JI Integr. Environ. Assess. Manag. PD JAN PY 2015 VL 11 IS 1 BP 5 EP 9 DI 10.1002/ieam.1587 PG 5 WC Environmental Sciences; Toxicology SC Environmental Sciences & Ecology; Toxicology GA CG8LN UT WOS:000353559300003 PM 25348557 ER PT J AU Rigg, DK Wacksman, MN Iannuzzi, J Baker, TF Adams, M Greeley, MS AF Rigg, David K. Wacksman, Mitch N. Iannuzzi, Jacqueline Baker, Tyler F. Adams, Marshall Greeley, Mark S., Jr. TI Assessing Ecological Risks to the Fish Community from Residual Coal Fly Ash in Watts Bar Reservoir, Tennessee SO INTEGRATED ENVIRONMENTAL ASSESSMENT AND MANAGEMENT LA English DT Article DE Arsenic; Selenium; Health metrics; Toxicity testing; Weight-of-evidence ID CLARIAS-BATRACHUS AB Extensive site-specific biological and environmental data were collected to support an evaluation of risks to the fish community in Watts Bar Reservoir from residual ash from the December 2008 Tennessee Valley Authority (TVA) Kingston ash release. This article describes the approach used and results of the risk assessment for the fish community, which consists of multiple measurement endpoints (measures of exposure and effects) for fish. The lines of evidence included 1) comparing postspill annual fish community assessments with nearby prespill data and data from other TVA reservoirs, 2) evaluating possible effects of exposures of fish eggs and larval fish to ash in controlled laboratory toxicity tests, 3) evaluating reproductive competence of field-exposed fish, 4) assessing individual fish health through physical examination, histopathology, and blood chemistry, 5) comparing fish tissue concentrations with literature-based critical body residues, and 6) comparing concentrations of ash-related contaminants in surface waters with US Environmental Protection Agency's (USEPA) Ambient Water Quality Standards for Fish and Aquatic Life. These measurement endpoints were treated as independent lines of evidence that were integrated into an overall weight-of-evidence estimate of risk to the fish community. Collectively, the data and analysis presented here indicate that ash and ash-related constituents pose negligible risks to the fish communities in Watts Bar Reservoir. This conclusion contradicts the predictions by some researchers immediately following the ash release of devastating effects on the aquatic ecology of Watts Bar Reservoir. The information presented in this article reaffirms the wisdom of carefully evaluating the evidence before predicting probable ecological effects of a major event such as the TVA Kingston ash release. This study demonstrates that a thorough and detailed investigation using multiple measurement endpoints is needed to properly evaluate ecological effects. Integr Environ Assess Manag 2015;11:88-101. (c) 2014 SETAC C1 [Rigg, David K.] ARCADIS, Clifton Pk, NY 12065 USA. [Wacksman, Mitch N.] ARCADIS, Portland, ME USA. [Iannuzzi, Jacqueline] ARCADIS, Annapolis, MD USA. [Baker, Tyler F.] Tennessee Valley Author, Chattanooga, TN USA. [Greeley, Mark S., Jr.] Oak Ridge Natl Lab, Oak Ridge, TN USA. RP Rigg, DK (reprint author), ARCADIS, Clifton Pk, NY 12065 USA. EM david.rigg@arcadis-us.com RI Greeley, Mark/D-2330-2016 OI Greeley, Mark/0000-0002-6088-5942 FU Tennessee Valley Authority (TVA) FX The authors thank the following individuals and agencies for their assistance with collecting, processing, and analyzing samples for this project: Teresa Matthews (fish bioaccumulation studies), Mark Bevelhimer (fish health studies), Mark Peterson, Allison Fortner, Oak Ridge National Laboratory, Environmental Standards, Pace Analytical Services, Restoration Services, Jacobs Engineering, US Fish and Wildlife Services, and Tennessee Wildlife Resources Agency. Funding for this project was provided by the Tennessee Valley Authority (TVA). NR 26 TC 3 Z9 3 U1 3 U2 8 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 1551-3777 EI 1551-3793 J9 INTEGR ENVIRON ASSES JI Integr. Environ. Assess. Manag. PD JAN PY 2015 VL 11 IS 1 BP 88 EP 101 DI 10.1002/ieam.1588 PG 14 WC Environmental Sciences; Toxicology SC Environmental Sciences & Ecology; Toxicology GA CG8LN UT WOS:000353559300011 PM 25346112 ER PT J AU Sample, BE Lowe, J Seeley, P Markin, M McCarthy, C Hansen, J Aly, AH AF Sample, Bradley E. Lowe, John Seeley, Paul Markin, Melanie McCarthy, Chris Hansen, Jim Aly, Alaa H. TI Depth of the Biologically Active Zone in Upland Habitats at the Hanford Site, Washington: Implications for Remediation and Ecological Risk Management SO INTEGRATED ENVIRONMENTAL ASSESSMENT AND MANAGEMENT LA English DT Article DE Biointrusion; Burrowing depth; Hanford Site; Rooting depth; Soil contamination ID FLORIDA HARVESTER ANT; NEST ARCHITECTURE; POGONOMYRMEX-BADIUS; SOCIOGENESIS; SOCIOMETRY; BARRIERS AB Soil invertebrates, mammals, and plants penetrate and exploit the surface soil layer (i.e., the biologically active zone) to varying depths. As the US Department of Energy remediates radioactive and hazardous wastes in soil at the Hanford Site, a site-specific definition of the biologically active zone is needed to identify the depth to which remedial actions should be taken to protect the environment and avoid excessive cleanup expenditures. This definition may then be considered in developing a point of compliance for remediation in accordance with existing regulations. Under the State of Washington Model Toxic Control Act (MTCA), the standard point of compliance for soil cleanup levels with unrestricted land use is 457cm (15ft) below ground surface. When institutional controls are required to control excavations to protect people, MTCA allows a conditional point of compliance to protect biological resources based on the depth of the biologically active zone. This study was undertaken to identify and bound the biologically active zone based on ecological resources present at the Hanford Site. Primary data were identified describing the depths to which ants, mammals, and plants may exploit the surface soil column at the Hanford Site and other comparable locations. The maximum depth observed for harvester ants (Pogonomyrmex spp.) was 270cm (8.9ft), with only trivial excavation below 244cm (8ft). Badgers (Taxidea taxus) are the deepest burrowing mammal at the Hanford Site, with maximum burrow depths of 230cm (7.6ft); all other mammals did not burrow below 122cm (4ft). Shrubs are the deepest rooting plants with rooting depths to 300cm (9.8ft) for antelope bitterbrush (Purshia tridentata). The 2 most abundant shrub species did not have roots deeper than 250cm (8.2ft). The deepest rooted forb had a maximum root depth of 240cm (7.9ft). All other forbs and grasses had rooting depths of 200cm (6.6ft) or less. These data indicate that the biologically active soil zone in the Hanford Central Plateau does not exceed 300cm (9.8ft), the maximum rooting depth for the deepest rooting plant. The maximum depth at which most other plant and animal species occur is substantially shallower. Spatial distribution and density of burrows and roots over depths were also evaluated. Although maximum excavation by harvester ants is 270cm (8.9ft), trivial volume of soil is excavated below 150cm (approximate to 5ft). Maximum rooting depths for all grasses, forbs, and the most abundant and deepest rooting shrubs are 300cm (9.8ft) or less. Most root biomass (>50-80%) is concentrated in the top 100cm (3.3ft), whereas at the maximum depth (9.8ft), only trace root biomass is present. Available data suggest a limited likelihood for significant transport of contaminants to the surface by plants at or below 244cm (8ft), and suggest that virtually all plants or animal species occurring on the Central Plateau have a negligible likelihood for transporting soil contaminants to the surface from depths at or below 305cm (10ft). Integr Environ Assess Manag 2015;11:150-160. (c) 2014 SETAC C1 [Sample, Bradley E.] Ecol Risk, Rancho Murieta, CA 95683 USA. [Lowe, John] CH2M HILL Plateau Remediat Co, Richland, WA USA. [Seeley, Paul] Cenibark Int, Richland, WA USA. [Markin, Melanie] CH2M Hill Inc, Sacramento, CA USA. [McCarthy, Chris] CH2M Hill Inc, Boston, MA USA. [Hansen, Jim] US DOE, Richland Operat Off, Richland, WA USA. [Aly, Alaa H.] INTERA, Richland, WA USA. RP Sample, BE (reprint author), Ecol Risk, Rancho Murieta, CA 95683 USA. EM bsample@ecorisk.com FU US Department of Energy; CH2M HILL Plateau Remediation Company FX Support for this analysis was provided by the US Department of Energy and the CH2M HILL Plateau Remediation Company. Much of this manuscript's content was reviewed by the regulatory agencies (USEPA and State of Washington Department of Ecology). Although this manuscript and its conclusions have not been endorsed by either agency, the manuscript benefited from excellent comments received from agencies staff. NR 33 TC 1 Z9 1 U1 1 U2 7 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 1551-3777 EI 1551-3793 J9 INTEGR ENVIRON ASSES JI Integr. Environ. Assess. Manag. PD JAN PY 2015 VL 11 IS 1 BP 150 EP 160 DI 10.1002/ieam.1581 PG 11 WC Environmental Sciences; Toxicology SC Environmental Sciences & Ecology; Toxicology GA CG8LN UT WOS:000353559300016 PM 25209119 ER PT J AU Duffin, AM Springer, KW Ward, JD Jarman, KD Robinson, JW Endres, MC Hart, GL Gonzalez, JJ Oropeza, D Russo, RE Willingham, DG Naes, BE Fahey, AJ Eiden, GC AF Duffin, Andrew M. Springer, Kellen W. Ward, Jesse D. Jarman, Kenneth D. Robinson, John W. Endres, Mackenzie C. Hart, Garret L. Gonzalez, Jhanis J. Oropeza, Dayana Russo, Richard E. Willingham, David G. Naes, Benjamin E. Fahey, Albert J. Eiden, Gregory C. TI Femtosecond laser ablation multicollector ICPMS analysis of uranium isotopes in NIST glass SO JOURNAL OF ANALYTICAL ATOMIC SPECTROMETRY LA English DT Article ID PLASMA-MASS SPECTROMETRY; TRANSPORT EFFICIENCIES; REFERENCE VALUES; MC-ICPMS; MS; PARTICLES; PLUTONIUM; RESOLUTION; AEROSOLS; STANDARD AB We utilized femtosecond laser ablation together with multi-collector inductively coupled plasma mass spectrometry to measure the uranium isotopic content of NIST 61x (x = 0, 2, 4, 6) glasses. The uranium content of these glasses is a linear two-component mixing between isotopically natural uranium and the isotopically depleted spike used in preparing the glasses. Laser ablation results match extremely well, generally within a few ppm, with solution analysis following sample dissolution and chemical separation. In addition to isotopic data, sample utilization efficiency measurements indicate that over 1% of ablated uranium atoms reach a mass spectrometer detector, making this technique extremely efficient. Laser sampling also allows for spatial analysis and our data indicate that rare uranium concentration inhomogeneities exist in NIST 616 glass. C1 [Duffin, Andrew M.; Springer, Kellen W.; Ward, Jesse D.; Jarman, Kenneth D.; Robinson, John W.; Endres, Mackenzie C.; Hart, Garret L.; Willingham, David G.; Naes, Benjamin E.; Eiden, Gregory C.] Pacific NW Natl Lab, Richland, WA 99352 USA. [Gonzalez, Jhanis J.; Oropeza, Dayana; Russo, Richard E.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Fahey, Albert J.] Naval Res Lab, Washington Dc, DC USA. RP Eiden, GC (reprint author), Pacific NW Natl Lab, Richland, WA 99352 USA. EM gregory.eiden@pnnl.gov RI Fahey, Albert/C-5611-2015; Jarman, Kenneth/B-6157-2011; OI Jarman, Kenneth/0000-0002-4396-9212; Willingham, David/0000-0002-7166-8994 FU National Nuclear Security Administration, Office of Defense Nuclear Nonproliferation Research and Development [DNN-RD/NA-22]; U.S. Department of Energy (DOE) [DE-AC05-75RLO1830]; Chemical Science Division, Office of Basic Energy Sciences; Defense Nuclear Nonproliferation Research and Development Office of the U.S. DOE at the Lawrence Berkeley National Laboratory [DE-AC02-05CH11231] FX The National Nuclear Security Administration, Office of Defense Nuclear Nonproliferation Research and Development, DNN-RD/NA-22, supported this work under an Interagency Agreement with the U.S. Department of Energy (DOE) under Contract DE-AC05-75RLO1830. Part of this work was supported by the Chemical Science Division, Office of Basic Energy Sciences and the Defense Nuclear Nonproliferation Research and Development Office of the U.S. DOE under contract number DE-AC02-05CH11231 at the Lawrence Berkeley National Laboratory. NR 36 TC 4 Z9 5 U1 6 U2 26 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 0267-9477 EI 1364-5544 J9 J ANAL ATOM SPECTROM JI J. Anal. At. Spectrom. PY 2015 VL 30 IS 5 BP 1100 EP 1107 DI 10.1039/c4ja00452c PG 8 WC Chemistry, Analytical; Spectroscopy SC Chemistry; Spectroscopy GA CH1FW UT WOS:000353767600010 ER PT J AU Hu, W Wang, T Yang, JL AF Hu, Wei Wang, Tian Yang, Jinlong TI Tunable Schottky contacts in hybrid graphene-phosphorene nanocomposites SO JOURNAL OF MATERIALS CHEMISTRY C LA English DT Article ID HEXAGONAL BORON-NITRIDE; GRAPHITIC CARBON NITRIDE; VISIBLE-LIGHT; AB-INITIO; BLACK PHOSPHORUS; POROUS SILICENE; THIN-FILMS; HETEROSTRUCTURES; TRANSISTORS; MOBILITY AB Combining the electronic structures of two-dimensional monolayers in ultrathin hybrid nanocomposites is expected to display new properties beyond their single components. Here, first-principles calculations are performed to study the structural and electronic properties of hybrid graphene and phosphorene nanocomposites. Our calculations show that weak van der Waals interactions dominate between graphene and phosphorene with their intrinsic electronic properties preserved. Furthermore, we found that as the interfacial distance decreases, the Dirac point of graphene moves from the conduction band to the valence band of phosphorene in hybrid graphene and phosphorene nanocomposites, inducing a transition from an n-type Schottky contact to a p-type Schottky contact at the graphene/phosphorene interface. C1 [Hu, Wei; Yang, Jinlong] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Computat Res Div, Berkeley, CA 94720 USA. [Hu, Wei] Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Anhui, Peoples R China. [Wang, Tian] Univ Sci & Technol China, Dept Precis Machinery & Precis Instrumentat, Hefei 230026, Anhui, Peoples R China. [Yang, Jinlong] Univ Sci & Technol China, Synerget Innovat Ctr Quantum Informat & Quantum P, Hefei 230026, Anhui, Peoples R China. RP Hu, W (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Computat Res Div, Berkeley, CA 94720 USA. EM whu@lbl.gov; jlyang@ustc.edu.cn RI Yang, Jinlong/D-3465-2009; OI Yang, Jinlong/0000-0002-5651-5340; Hu, Wei/0000-0001-9629-2121 FU National Key Basic Research Program [2011CB921404]; NSFC [21421063, 91021004, 21233007]; Chinese Academy of Sciences (CAS) [XDB01020300]; USTCSCC, SCCAS, Tianjin; Shanghai Supercomputer Centers; Scientific Discovery through Advanced Computing (SciDAC) Program - U.S. Department of Energy, Office of Science, Advanced Scientific Computing Research and Basic Energy Sciences FX This work was partially supported by the National Key Basic Research Program (2011CB921404), by NSFC (21421063, 91021004, 21233007), by Chinese Academy of Sciences (CAS) (XDB01020300), and by USTCSCC, SCCAS, Tianjin, and Shanghai Supercomputer Centers. This work is also partially supported by the Scientific Discovery through Advanced Computing (SciDAC) Program funded by U.S. Department of Energy, Office of Science, Advanced Scientific Computing Research and Basic Energy Sciences (W. H.). We thank the National Energy Research Scientific Computing (NERSC) center for the computational resources. NR 86 TC 25 Z9 25 U1 4 U2 59 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7526 EI 2050-7534 J9 J MATER CHEM C JI J. Mater. Chem. C PY 2015 VL 3 IS 18 BP 4756 EP 4761 DI 10.1039/c5tc00759c PG 6 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA CH1GB UT WOS:000353768100022 ER PT S AU Bochove, E Neschke, B Nair, N Delgado, P Braiman, Y AF Bochove, Erik Neschke, Brendan Nair, Niketh Delgado, Paul Braiman, Yehuda BE Kudryashov, AV Paxton, AH Ilchenko, VS Aschke, L Washio, K TI Phase dynamics of high radiance fiber laser arrays with active phase control SO LASER RESONATORS, MICRORESONATORS, AND BEAM CONTROL XVII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Laser Resonators, Microresonators, and Beam Control XVII CY FEB 09-12, 2015 CL San Francisco, CA SP SPIE DE Laser Arrays; Coherent Arrays; Active Feedback ID COHERENT BEAM AB The existing model of the LOCSET technique for the active phase synchronization of fiber laser arrays (T. Shay, Opt. Express, 2006) is extended to include relevant physical properties of the system, such as inherent optical path differences (OPD), line-width and group velocity dispersion (GVD), and we also include phase "jitter" of the master oscillator's output in the model, which in experiments is implemented to induce spectral broadening for suppression of nonlinear frequency conversion. Linearization of the phase error signal, which incorrectly predicts convergence to a synchronous equilibrium state, is not performed. Instead, the closed-loop control dynamics are shown to be described by differential equations of Kuramoto type when phase corrector response dynamics are negligible. Linear stability analysis indicates that there is always one and no more than one dynamically stable state. The latter is shown to be normally synchronous, except when strong "jitter" is applied. A Liapounov function is found as subject to the validity of certain symmetry conditions. C1 [Bochove, Erik] US Air Force, Res Lab, Directed Energy Directorate, Kirtland AFB, NM 87117 USA. [Neschke, Brendan; Nair, Niketh; Braiman, Yehuda] Univ Tennessee, Dept Mech Aerosp & Biomed Engn, Knoxville, TN 37996 USA. [Neschke, Brendan; Nair, Niketh; Braiman, Yehuda] Oak Ridge Natl Lab, Ctr Engn Sci Adv Res, Comp Sci & Math Div, Oak Ridge, TN 37831 USA. [Delgado, Paul] Univ Texas El Paso, Dept Computat Sci, El Paso, TX 79924 USA. [Nair, Niketh; Delgado, Paul] LEIDOS, Albuquerque, NM 87106 USA. RP Bochove, E (reprint author), US Air Force, Res Lab, Directed Energy Directorate, Kirtland AFB, NM 87117 USA. NR 10 TC 0 Z9 0 U1 1 U2 1 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-1-62841-433-2 J9 PROC SPIE PY 2015 VL 9343 AR 93431C DI 10.1117/12.2080538 PG 15 WC Engineering, Electrical & Electronic; Optics; Physics, Applied SC Engineering; Optics; Physics GA BC6AK UT WOS:000353695900027 ER PT S AU Nair, N Bochove, EJ Aceves, AB Zunoubi, MR Braiman, Y AF Nair, Niketh Bochove, Erik J. Aceves, Alejandro B. Zunoubi, Mohammad R. Braiman, Yehuda BE Kudryashov, AV Paxton, AH Ilchenko, VS Aschke, L Washio, K TI Resonator modes and mode dynamics for an external cavity-coupled laser array SO LASER RESONATORS, MICRORESONATORS, AND BEAM CONTROL XVII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Laser Resonators, Microresonators, and Beam Control XVII CY FEB 09-12, 2015 CL San Francisco, CA SP SPIE DE Coupled mode theory; coherent beam combining; laser arrays; passive phasing ID SEMICONDUCTOR-LASERS; MULTICORE FIBER; WAVE-GUIDES; EIGENMODES; FEEDBACK AB Employing a Fox-Li approach, we derived the cold-cavity mode structure and a coupled mode theory for a phased array of N single-transverse-mode active waveguides with feedback from an external cavity. We applied the analysis to a system with arbitrary laser lengths, external cavity design and coupling strengths to the external cavity. The entire system was treated as a single resonator. The effect of the external cavity was modeled by a set of boundary conditions expressed by an N-by-N frequency-dependent matrix relation between incident and reflected fields at the interface with the external cavity. The coupled mode theory can be adapted to various types of gain media and internal and external cavity designs. C1 [Nair, Niketh; Braiman, Yehuda] Oak Ridge Natl Lab, Div Math & Comp Sci, Oak Ridge, TN 37831 USA. [Nair, Niketh; Braiman, Yehuda] Univ Tennessee, Dept Engn Mech, Knoxville, TN 37996 USA. [Bochove, Erik J.] US Air Force, Res Lab, Directed Energy Directorate, Kirtland AFB, NM 87117 USA. [Aceves, Alejandro B.] So Methodist Univ, Dept Math, Dallas, TX 75275 USA. SUNY Coll New Paltz, Dept Elect & Comp Engn, New Paltz, NY 12561 USA. RP Nair, N (reprint author), Oak Ridge Natl Lab, Div Math & Comp Sci, Oak Ridge, TN 37831 USA. EM nnair@vols.utk.edu NR 37 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 978-1-62841-433-2 J9 PROC SPIE PY 2015 VL 9343 AR 93431D DI 10.1117/12.2080569 PG 11 WC Engineering, Electrical & Electronic; Optics; Physics, Applied SC Engineering; Optics; Physics GA BC6AK UT WOS:000353695900028 ER PT S AU Yahagi, Y Harteneck, B Cabrini, S Schmidt, H AF Yahagi, Yu Harteneck, Bruce Cabrini, Stefano Schmidt, Holger BE Adibi, A Lin, SY Scherer, A TI Control of the magnetization dynamics in patterned nanostructures with magnetoelastic coupling SO PHOTONIC AND PHONONIC PROPERTIES OF ENGINEERED NANOSTRUCTURES V SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Photonic and Phononic Properties of Engineered Nanostructures V CY FEB 09-12, 2015 CL San Francisco, CA SP SPIE DE phononic crystal; magnetization dynamics; time-resolved MOKE; magnetoelastic coupling; spin waves; surface acoustic waves AB We review the influence of the magnetoelastic coupling with surface acoustic waves (SAWs) on the dynamic magnetic response of a periodic nanomagnet array. In addition to exciting the magnetization precession, an ultrafast laser pulse generates multiple SAW modes whose frequencies are determined by the array pitch. As a result, strong pinning of the magnetization precession frequency at the crossover points with the SAWs is observed over an extended field range. The complex spin wave spectrum can be analyzed in frequency and momentum spaces using finite element analysis emulating generation of SAWs. The magnetic response of the nanomagnets was then correctly reproduced with micromagnetic simulations taking into account additional magnetoelastic energy terms. This finding demonstrates control of the nanomagnet dynamics with the array geometry via magnetoelastic coupling, even when the magnetostatic interaction between the magnets is negligible. C1 [Yahagi, Yu; Schmidt, Holger] Univ Calif Santa Cruz, Sch Engn, Santa Cruz, CA 95064 USA. [Harteneck, Bruce; Cabrini, Stefano] Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA. RP Yahagi, Y (reprint author), Univ Calif Santa Cruz, Sch Engn, 1156 High St, Santa Cruz, CA 95064 USA. EM hsehmidt@soe.uese.edu NR 29 TC 0 Z9 0 U1 2 U2 13 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-1-62841-461-5 J9 PROC SPIE PY 2015 VL 9371 AR 93711O DI 10.1117/12.2084978 PG 8 WC Engineering, Electrical & Electronic; Optics; Physics, Applied SC Engineering; Optics; Physics GA BC6AO UT WOS:000353706000018 ER PT J AU Lara-Garcia, HA Alcantar-Vazquez, B Duan, YH Pfeiffer, H AF Lara-Garcia, Hugo A. Alcantar-Vazquez, Brenda Duan, Yuhua Pfeiffer, Heriberto TI Water steam effect during high CO2 chemisorption in lithium cuprate (Li2CuO2) at moderate temperatures: experimental and theoretical evidence SO RSC ADVANCES LA English DT Article ID 30-80 DEGREES-C; CARBON-DIOXIDE; CAPTURE PROPERTIES; VAPOR ADDITION; ABSORPTION; ZIRCONATE; SEQUESTRATION; ORTHOSILICATE; SORPTION; KINETICS AB Li2CuO2 was evaluated as a CO2 captor at moderate temperatures, using water vapor in the gas flow. Different water vapor sorption experiments were performed using N-2 or CO2 as carrier gases. If N-2 was used as carrier gas, it was evidenced that Li2CuO2 is able to trap water physically and chemically, producing in the second case Li-OH superficial species. Moreover, when CO2 was used as carrier gas, Li2CuO2 continued trapping water, as in the previous case, but in this case CO2 was mainly trapped, forming Li2CO3 and CuO phases. Additionally, the microstructure changes importantly when CO2 and H2O are chemically trapped in Li2CuO2. Li2CO3 and CuO seemed to segregate changing the morphology and the specific surface area. The Li2CuO2 sample was able to capture up to 6.7 mmoles of CO2 per gram of ceramic at 80 degrees C, a considerably high CO2 amount. Furthermore, all these experiments were theoretically supported by different thermodynamic calculations. Experimental and theoretical results show that H2O acts as a catalytic intermediate, diminishing the activation energy of the whole CO2 chemisorption process. Therefore, the presence of water vapor strongly favored the CO2 chemisorption on Li2CuO2 at moderate temperatures (30-80 degrees C). C1 [Lara-Garcia, Hugo A.; Alcantar-Vazquez, Brenda; Pfeiffer, Heriberto] Univ Nacl Autonoma Mexico, Inst Invest Mat, Mexico City 04510, DF, Mexico. [Duan, Yuhua] US DOE, Natl Energy Technol Lab, Pittsburgh, PA 15236 USA. RP Pfeiffer, H (reprint author), Univ Nacl Autonoma Mexico, Inst Invest Mat, Circuito Exterior S-N Cd Univ,Del Coyoacan, Mexico City 04510, DF, Mexico. EM pfeiffer@iim.unam.mx FU project PAPIIT-UNAM [IN-102313]; project SENER-CONACYT [150358]; CONACYT FX This work was financially supported by the projects PAPIIT-UNAM (IN-102313) and SENER-CONACYT (150358). H. Lara-Garcia thanks CONACYT for financial support. The authors thank to Adriana Tejeda and Josue Romero-Ibarra for technical help. NR 62 TC 8 Z9 8 U1 3 U2 15 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2046-2069 J9 RSC ADV JI RSC Adv. PY 2015 VL 5 IS 43 BP 34157 EP 34165 DI 10.1039/c5ra03580e PG 9 WC Chemistry, Multidisciplinary SC Chemistry GA CG3GR UT WOS:000353167500056 ER PT J AU Spafford, KL Vetter, JS AF Spafford, Kyle L. Vetter, Jeffrey S. TI Automated Design Space Exploration with Aspen SO SCIENTIFIC PROGRAMMING LA English DT Article ID PARALLEL COMPUTATION; ALGORITHM; MODEL; OPTIMIZATION; FUTURE AB Architects and applications scientists often use performance models to explore a multidimensional design space of architectural characteristics, algorithm designs, and application parameters. With traditional performance modeling tools, these explorations forced users to first develop a performance model and then repeatedly evaluate and analyze the model manually. These manual investigations proved laborious and error prone. More importantly, the complexity of this traditional process often forced users to simplify their investigations. To address this challenge of design space exploration, we extend our Aspen (Abstract Scalable Performance Engineering Notation) language with three new language constructs: user-defined resources, parameter ranges, and a collection of costs in the abstract machine model. Then, we use these constructs to enable automated design space exploration via a nonlinear optimization solver. We show how four interesting classes of design space exploration scenarios can be derived from Aspen models and formulated as pure nonlinear programs. The analysis tools are demonstrated using examples based on Aspen models for a three-dimensional Fast Fourier Transform, the CoMD molecular dynamics proxy application, and the DARPA Streaming Sensor Challenge Problem. Our results show that this approach can compose and solve arbitrary performance modeling questions quickly and rigorously when compared to the traditional manual approach. C1 [Spafford, Kyle L.; Vetter, Jeffrey S.] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. RP Vetter, JS (reprint author), Oak Ridge Natl Lab, One Bethel Valley Rd,Bldg 5100,MS-6173, Oak Ridge, TN 37831 USA. EM vetter@computer.org FU Office of Advanced Scientific Computing Research in U.S. Department of Energy; DARPA [HR0011-10-9-0008]; U.S. Government [DE-AC05-00OR22725] FX This research is sponsored by the Office of Advanced Scientific Computing Research in the U.S. Department of Energy and DARPA Contract HR0011-10-9-0008. The paper has been authored by Oak Ridge National Laboratory, which is managed by UT-Battelle, LLC under Contract DE-AC05-00OR22725 to the U.S. Government. Accordingly, the U.S. Government retains a nonexclusive, royalty-free license to publish or reproduce the published form of this contribution, or allow others to do so, for U.S. Government purposes. NR 42 TC 0 Z9 0 U1 0 U2 1 PU HINDAWI PUBLISHING CORP PI NEW YORK PA 315 MADISON AVE 3RD FLR, STE 3070, NEW YORK, NY 10017 USA SN 1058-9244 EI 1875-919X J9 SCI PROGRAMMING-NETH JI Sci. Program. PY 2015 BP 1 EP 10 AR 157305 DI 10.1155/2015/157305 PG 10 WC Computer Science, Software Engineering SC Computer Science GA CH2ER UT WOS:000353839000001 ER PT J AU Cai, ZQ Falgout, R Zhang, S AF Cai, Zhiqiang Falgout, Rob Zhang, Shun TI DIV FIRST-ORDER SYSTEM LL* (FOSLL*) FOR SECOND-ORDER ELLIPTIC PARTIAL DIFFERENTIAL EQUATIONS SO SIAM JOURNAL ON NUMERICAL ANALYSIS LA English DT Article DE LL* method; least-squares method; a priori error estimate; a posteriori error estimate; elliptic equations ID LEAST-SQUARES AB The first-order system LL* (FOSLL*) approach for general second-order elliptic partial differential equations was proposed and analyzed in [Z. Cai et al., SIAM J. Numer. Anal., 39 (2001), pp. 1418-1445], in order to retain the full efficiency of the L-2 norm first-order system least-squares (FOSLS) approach while exhibiting the generality of the inverse-norm FOSLS approach. The FOSLL* approach of Cai et al. was applied to the div-curl system with added slack variables, and hence it is quite complicated. In this paper, we apply the FOSLL* approach to the div system and establish its well-posedness. For the corresponding finite element approximation, we obtain a quasi-optimal a priori error bound under the same regularity assumption as the standard Galerkin method, but without the restriction to sufficiently small mesh size. Unlike the FOSLS approach, the FOSLL* approach does not have a free a posteriori error estimator. We then propose an explicit residual error estimator and establish its reliability and efficiency bounds. C1 [Cai, Zhiqiang] Purdue Univ, Dept Math, W Lafayette, IN 47907 USA. [Falgout, Rob] Lawrence Livermore Natl Lab, Ctr Appl Sci Comp, Livermore, CA 94551 USA. [Zhang, Shun] City Univ Hong Kong, Dept Math, Hong Kong, Hong Kong, Peoples R China. RP Cai, ZQ (reprint author), Purdue Univ, Dept Math, W Lafayette, IN 47907 USA. EM caiz@purdue.edu; falgout2@llnl.gov; shun.zhang@cityu.edu.hk RI Zhang, Shun/J-5972-2016 OI Zhang, Shun/0000-0001-6235-0362 FU U.S. Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07NA27344 (LLNL-JRNL-645325)]; National Science Foundation [DMS-1217081]; Research Grants Council of the Hong Kong SAR, China, under GRF grant [11303914, CityU 9042090] FX This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under contract DE-AC52-07NA27344 (LLNL-JRNL-645325). The research was supported in part by the National Science Foundation under grant DMS-1217081 and the Research Grants Council of the Hong Kong SAR, China, under GRF grant project 11303914, CityU 9042090. NR 18 TC 2 Z9 2 U1 0 U2 1 PU SIAM PUBLICATIONS PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA SN 0036-1429 EI 1095-7170 J9 SIAM J NUMER ANAL JI SIAM J. Numer. Anal. PY 2015 VL 53 IS 1 BP 405 EP 420 DI 10.1137/140971890 PG 16 WC Mathematics, Applied SC Mathematics GA CH2GW UT WOS:000353844700019 ER PT J AU Jones, BH Martinez, AM Wheeler, JS Spoerke, ED AF Jones, Brad H. Martinez, Alina M. Wheeler, Jill S. Spoerke, Erik D. TI Surfactant-induced assembly of enzymatically-stable peptide hydrogels SO SOFT MATTER LA English DT Article ID SODIUM DODECYL-SULFATE; AMYLOID-BETA PEPTIDE; CRITICAL MICELLE CONCENTRATION; CONFORMATIONAL TRANSITION; POLY(L-GLUTAMIC ACID); AQUEOUS-SOLUTION; CIRCULAR-DICHROISM; CHAIN-LENGTH; ALPHA-HELIX; CATIONIC SURFACTANTS AB The secondary structure of peptides in the presence of interacting additives is an important topic of study, having implications in the application of peptide science to a broad range of modern technologies. Surfactants constitute a class of biologically relevant compounds that are known to influence both peptide conformation and aggregation or assembly. We have characterized the secondary structure of a linear nonapeptide composed of a hydrophobic alanine/phenylalanine core flanked by hydrophilic acid/amine units. We show that the anionic surfactant sodium dodecyl sulfate (SDS) induces the formation of beta-sheets and macroscopic gelation in this otherwise unstructured peptide. Through comparison to related additives, we propose that SDS-induced secondary structure formation is the result of amphiphilicity created by electrostatic binding of SDS to the peptide. In addition, we demonstrate a novel utility of surfactants in manipulating and stabilizing peptide nanostructures. SDS is used to simultaneously induce secondary structure in a peptide and to inhibit the activity of a model enzyme, resulting in a peptide hydrogel that is impervious to enzymatic degradation. These results complement our understanding of the behavior of peptides in the presence of interacting secondary molecules and provide new potential pathways for programmable organization of peptides by the addition of such components. C1 [Jones, Brad H.; Martinez, Alina M.; Wheeler, Jill S.; Spoerke, Erik D.] Sandia Natl Labs, Elect Opt & Nano Mat, Albuquerque, NM 87185 USA. RP Spoerke, ED (reprint author), Sandia Natl Labs, Elect Opt & Nano Mat, POB 5800,MS 1411, Albuquerque, NM 87185 USA. EM edspoer@sandia.gov FU U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering [KC0203010]; US Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX We gratefully acknowledge Ken Sherrell and the University of New Mexico MS facility and Dr James Hochrein and Lance Miller for performing MS. We gratefully acknowledge Dr Nelson Bell for assistance with rheological experiments. We also thank Dr George Bachand for insightful discussion. This research was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering, Project KC0203010. Sandia National Laboratories is a multi-program laboratory operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the US Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000. NR 82 TC 2 Z9 2 U1 10 U2 35 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1744-683X EI 1744-6848 J9 SOFT MATTER JI Soft Matter PY 2015 VL 11 IS 18 BP 3572 EP 3580 DI 10.1039/c5sm00522a PG 9 WC Chemistry, Physical; Materials Science, Multidisciplinary; Physics, Multidisciplinary; Polymer Science SC Chemistry; Materials Science; Physics; Polymer Science GA CG9SI UT WOS:000353660000008 PM 25853589 ER PT J AU Gunaratne, KDD Prabhakaran, V Ibrahim, YM Norheim, RV Johnson, GE Laskin, J AF Gunaratne, K. Don D. Prabhakaran, Venkateshkumar Ibrahim, Yehia M. Norheim, Randolph V. Johnson, Grant E. Laskin, Julia TI Design and performance of a high-flux electrospray ionization source for ion soft landing SO ANALYST LA English DT Article ID MASS-SELECTED IONS; SIZE-SELECTED CLUSTERS; ASSEMBLED MONOLAYER SURFACES; LANDED PROTEIN VOLTAMMETRY; SUPPORTED METAL-CLUSTERS; IN-SITU; CHEMICAL-MODIFICATION; BIOMOLECULAR IONS; PREPARATIVE SOFT; SIMS ANALYSIS AB We report the design and evaluation of a new high-intensity electrospray ionization source for ion soft-landing experiments. The source incorporates a dual ion funnel, which enables operation with a higher gas load through an expanded diameter heated inlet into the additional first region of differential pumping. This capability allowed us to examine the effect of the inner diameter (ID) of the heated stainless steel inlet on the total ion current transmitted through the dual funnel interface and, more importantly, the mass-selected ion current delivered to the deposition target. The ion transmission of the dual funnel is similar to the transmission of the single funnel used in our previous soft landing studies. However, substantially higher ion currents were obtained using larger ID heated inlets and an orthogonal inlet geometry, in which the heated inlet was positioned perpendicular to the direction of ion propagation through the instrument. The highest ion currents were obtained using the orthogonal geometry and a 1.4 mm ID heated inlet. The corresponding stable deposition rate of similar to 1 mu g of mass-selected ions per day will facilitate future studies focused on the controlled deposition of complex molecules on substrates for studies in catalysis, energy storage, and self-assembly. C1 [Gunaratne, K. Don D.; Prabhakaran, Venkateshkumar; Johnson, Grant E.; Laskin, Julia] Pacific NW Natl Lab, Div Phys Sci, Richland, WA 99352 USA. [Ibrahim, Yehia M.; Norheim, Randolph V.] Pacific NW Natl Lab, Biol Sci Div, Richland, WA 99352 USA. [Ibrahim, Yehia M.; Norheim, Randolph V.] Pacific NW Natl Lab, Environm Mol Sci Lab, Richland, WA 99352 USA. RP Laskin, J (reprint author), Pacific NW Natl Lab, Div Phys Sci, POB 999,MSIN K8-88, Richland, WA 99352 USA. EM Julia.Laskin@pnnl.gov RI Prabhakaran, Venkateshkumar/C-5023-2009; OI Prabhakaran, Venkateshkumar/0000-0001-6692-6488; Laskin, Julia/0000-0002-4533-9644; Johnson, Grant/0000-0003-3352-4444 FU US Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences Biosciences; DOE's Office of Biological and Environmental Research FX This work was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences & Biosciences and performed in EMSL, a national scientific user facility sponsored by the DOE's Office of Biological and Environmental Research and located at the Pacific Northwest National Laboratory (PNNL). PNNL is operated by Battelle for the U.S. DOE. NR 76 TC 11 Z9 11 U1 5 U2 35 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 0003-2654 EI 1364-5528 J9 ANALYST JI Analyst PY 2015 VL 140 IS 9 BP 2957 EP 2963 DI 10.1039/c5an00220f PG 7 WC Chemistry, Analytical SC Chemistry GA CG3CK UT WOS:000353154400004 PM 25800562 ER PT J AU Marelle, L Raut, JC Thomas, JL Law, KS Quennehen, B Ancellet, G Pelon, J Schwarzenboeck, A Fast, JD AF Marelle, L. Raut, J. -C. Thomas, J. L. Law, K. S. Quennehen, B. Ancellet, G. Pelon, J. Schwarzenboeck, A. Fast, J. D. TI Transport of anthropogenic and biomass burning aerosols from Europe to the Arctic during spring 2008 SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID POLARCAT SUMMER CAMPAIGN; NORTH-AMERICA; AIR-POLLUTION; ATMOSPHERIC AEROSOLS; CLOUD MICROPHYSICS; OPTICAL-PROPERTIES; ORGANIC-COMPOUNDS; BLACK CARBON; MODEL; EMISSIONS AB During the POLARCAT-France airborne campaign in April 2008, pollution originating from anthropogenic and biomass burning emissions was measured in the European Arctic. We compare these aircraft measurements with simulations using the WRF-Chem model to investigate model representation of aerosols transported from Europe to the Arctic. Modeled PM2.5 is evaluated using European Monitoring and Evaluation Programme (EMEP) measurements in source regions and POLARCAT aircraft measurements in the Scandinavian Arctic. Total PM2.5 agrees well with the measurements, although the model overestimates nitrate and underestimates organic carbon in source regions. Using WRF-Chem in combination with the Lagrangian model FLEXPART-WRF, we find that during the campaign the research aircraft sampled two different types of European plumes: mixed anthropogenic and fire plumes from eastern Europe and Russia transported below 2 km, and anthropogenic plumes from central Europe uplifted by warm conveyor belt circulations to 5-6 km. Both modeled plume types had undergone significant wet scavenging (> 50% PM10) during transport. Modeled aerosol vertical distributions and optical properties below the aircraft are evaluated in the Arctic using airborne lidar measurements. Model results show that the pollution event transported aerosols into the Arctic (> 66.6 degrees N) for a 4-day period. During this 4-day period, biomass burning emissions have the strongest influence on concentrations between 2.5 and 3 km altitudes, while European anthropogenic emissions influence aerosols at both lower (similar to 1.5 km) and higher altitudes (similar to 4.5 km). As a proportion of PM2.5, modeled black carbon and SO4= concentrations are more enhanced near the surface in anthropogenic plumes. The European plumes sampled during the POLARCAT-France campaign were transported over the region of springtime snow cover in northern Scandinavia, where they had a significant local atmospheric warming effect. We find that, during this transport event, the average modeled top-of-atmosphere (TOA) shortwave direct and semi-direct radiative effect (DSRE) north of 60 degrees N over snow and ice-covered surfaces reaches +0.58W m(-2), peaking at +3.3W m(-2) at noon over Scandinavia and Finland. C1 [Marelle, L.; Raut, J. -C.; Thomas, J. L.; Law, K. S.; Quennehen, B.; Ancellet, G.; Pelon, J.] Univ Paris 06, Sorbonne Univ, Paris, France. [Marelle, L.; Raut, J. -C.; Thomas, J. L.; Law, K. S.; Quennehen, B.; Ancellet, G.; Pelon, J.] Univ Versailles St Quentin, Paris, France. [Marelle, L.; Raut, J. -C.; Thomas, J. L.; Law, K. S.; Quennehen, B.; Ancellet, G.; Pelon, J.] CNRS, INSU, LATMOS, IPSL, Paris, France. [Marelle, L.] TOTAL SA DS, F-92078 Paris, France. [Schwarzenboeck, A.] Univ Clermont Ferrand, CNRS, UMR6016, Lab Meteorol Phys, Aubiere, France. [Fast, J. D.] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Marelle, L (reprint author), Univ Paris 06, Sorbonne Univ, Paris, France. EM louis.marelle@latmos.ipsl.fr RI Raut, Jean-Christophe/G-3946-2016; OI Raut, Jean-Christophe/0000-0002-3552-2437 FU French research agency ANR Climate Impacts of Short-Lived Pollutants and Methane in the Arctic (CLIMSLIP) project; CNRS/LEFE; ANR "Programme d'Investissements d'Avenir" [ANR-10-LABX-0018]; Total; ANR; CNES; CNRS/INSU; IPEV FX This study was supported by the French research agency ANR Climate Impacts of Short-Lived Pollutants and Methane in the Arctic (CLIMSLIP) project and CNRS/LEFE. We also acknowledge support from the ANR "Programme d'Investissements d'Avenir" (grant no. ANR-10-LABX-0018). Financial support for this work was provided by Total. The UMS SAFIRE is acknowledged for supporting the ATR-42 aircraft deployment and for providing the aircraft meteorological data. The POLARCAT-FRANCE project was supported by ANR, CNES, CNRS/INSU, and IPEV. We thank Jerome Brioude (CIRES) for the development of FLEXPART-WRF. We thank the EDGAR team for compiling the HTAPv2 emissions (http://edgar.jrc.ec.europa.eu/htap_v2/index.php?SECURE=123). We acknowledge the E-OBS data set from the EU-FP6 project ENSEMBLES (http://ensembles-eu.metoffice.com) and the data providers in the ECA&D project (http://www.ecad.eu). Computing resources were provided by the IPSL CICLAD/CLIMSERV mesocenter. NR 82 TC 3 Z9 3 U1 4 U2 25 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1680-7316 EI 1680-7324 J9 ATMOS CHEM PHYS JI Atmos. Chem. Phys. PY 2015 VL 15 IS 7 BP 3831 EP 3850 DI 10.5194/acp-15-3831-2015 PG 20 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA CG0LF UT WOS:000352957400013 ER PT J AU Drewniak, BA Mishra, U Song, J Prell, J Kotamarthi, VR AF Drewniak, B. A. Mishra, U. Song, J. Prell, J. Kotamarthi, V. R. TI Modeling the impact of agricultural land use and management on US carbon budgets SO BIOGEOSCIENCES LA English DT Article ID SOIL ORGANIC-CARBON; RESIDUE REMOVAL; NITROGEN-FERTILIZATION; UNITED-STATES; CORN STOVER; CROP; SEQUESTRATION; DYNAMICS; TILLAGE; CLIMATE AB Cultivation of the terrestrial land surface can create either a source or sink of atmospheric CO2, depending on land management practices. The Community Land Model (CLM) provides a useful tool for exploring how land use and management impact the soil carbon pool at regional to global scales. CLM was recently updated to include representation of managed lands growing maize, soybean, and spring wheat. In this study, CLM-Crop is used to investigate the impacts of various management practices, including fertilizer use and differential rates of crop residue removal, on the soil organic carbon (SOC) storage of croplands in the continental United States over approximately a 170-year period. Results indicate that total US SOC stocks have already lost over 8 Pg C (10 %) due to land cultivation practices (e.g., fertilizer application, cultivar choice, and residue removal), compared to a land surface composed of native vegetation (i.e., grasslands). After long periods of cultivation, individual subgrids (the equivalent of a field plot) growing maize and soybean lost up to 65% of the carbon stored compared to a grassland site. Crop residue management showed the greatest effect on soil carbon storage, with low and medium residue returns resulting in additional losses of 5 and 3.5 %, respectively, in US carbon storage, while plots with high residue returns stored 2% more carbon. Nitrogenous fertilizer can alter the amount of soil carbon stocks significantly. Under current levels of crop residue return, not applying fertilizer resulted in a 5% loss of soil carbon. Our simulations indicate that disturbance through cultivation will always result in a loss of soil carbon, and management practices will have a large influence on the magnitude of SOC loss. C1 [Drewniak, B. A.; Mishra, U.; Prell, J.; Kotamarthi, V. R.] Argonne Natl Lab, Environm Sci Div, Argonne, IL 60439 USA. [Song, J.] No Illinois Univ, Dept Geog, De Kalb, IL 60115 USA. RP Drewniak, BA (reprint author), Argonne Natl Lab, Environm Sci Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM bbye@anl.gov FU US Department of Energy (DOE), Office of Science [DE-AC02-06CH11357]; Office of Science, under DOE [DE-AC02-05CH11231] FX This work was supported by the US Department of Energy (DOE), Office of Science, under contract DE-AC02-06CH11357. Numerical simulations were performed with resources provided by the National Energy Research Scientific Computing Center, supported by the Office of Science, under DOE contract DE-AC02-05CH11231. NR 67 TC 3 Z9 3 U1 3 U2 25 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1726-4170 EI 1726-4189 J9 BIOGEOSCIENCES JI Biogeosciences PY 2015 VL 12 IS 7 BP 2119 EP 2129 DI 10.5194/bg-12-2119-2015 PG 11 WC Ecology; Geosciences, Multidisciplinary SC Environmental Sciences & Ecology; Geology GA CG0LP UT WOS:000352958400005 ER PT J AU Zhao, JM Mu, LQ Qi, YR Hu, YS Liu, HZ Dai, S AF Zhao, Junmei Mu, Linqin Qi, Yuruo Hu, Yong-Sheng Liu, Huizhou Dai, Sheng TI A phase-transfer assisted solvo-thermal strategy for low-temperature synthesis of Na-3(VO1-xPO4)(2)F1+2x cathodes for sodium-ion batteries SO CHEMICAL COMMUNICATIONS LA English DT Article ID ENERGY-STORAGE; LITHIUM-ION; ELECTROCHEMICAL PERFORMANCE; NA3V2(PO4)(2)F-3 CATHODE; INSERTION PROPERTIES; POSITIVE ELECTRODE; IRON PHOSPHATE; FLUOROPHOSPHATE; NA3V2O2X(PO4)(2)F3-2X; MECHANISM AB We demonstrate that a series of high-performance cathode materials, sodium vanadium polyanionic compounds, Na-3(VO1-xPO4)(2)F1+2x (x = 0, 0.5 and 1), can be synthesized by a phase-transfer assisted solvo-thermal strategy at a rather low temperature (80-140 degrees C) in one simple step, exhibiting a high Na storage capacity of ca. 120 mA h g(-1) and excellent cycling performance. This study makes a significant step to extend this strategy to the synthesis of functional materials from simple binary to complex multicomponent compounds. C1 [Zhao, Junmei; Qi, Yuruo; Liu, Huizhou] Chinese Acad Sci, Inst Proc Engn, Key Lab Green Proc & Engn, Beijing 100190, Peoples R China. [Zhao, Junmei; Dai, Sheng] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. [Mu, Linqin; Hu, Yong-Sheng] Chinese Acad Sci, Inst Phys, Beijing Natl Lab Condensed Matter Phys, Beijing 100190, Peoples R China. RP Zhao, JM (reprint author), Chinese Acad Sci, Inst Proc Engn, Key Lab Green Proc & Engn, Beijing 100190, Peoples R China. EM jmzhao@ipe.ac.cn; hzliu@ipe.ac.cn RI Dai, Sheng/K-8411-2015; Hu, Yong-Sheng/H-1177-2011 OI Dai, Sheng/0000-0002-8046-3931; Hu, Yong-Sheng/0000-0002-8430-6474 FU Beijing Natural Science Foundation [2142030, 51222210]; "973" Projects [2012CB932900]; State Scholarship Fund from China Scholarship Council; U.S. Department of Energy's Office of Basic Energy Science, Division of Materials Sciences and Engineering FX This work was supported by Beijing Natural Science Foundation (2142030 and 51222210), and "973" Projects (2012CB932900) and by the State Scholarship Fund from China Scholarship Council. SD was supported by the U.S. Department of Energy's Office of Basic Energy Science, Division of Materials Sciences and Engineering. NR 39 TC 10 Z9 10 U1 11 U2 75 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1359-7345 EI 1364-548X J9 CHEM COMMUN JI Chem. Commun. PY 2015 VL 51 IS 33 BP 7160 EP 7163 DI 10.1039/c5cc01504a PG 4 WC Chemistry, Multidisciplinary SC Chemistry GA CF9DU UT WOS:000352863600018 PM 25812049 ER PT J AU Voiry, D Mohite, A Chhowalla, M AF Voiry, Damien Mohite, Aditya Chhowalla, Manish TI Phase engineering of transition metal dichalcogenides SO CHEMICAL SOCIETY REVIEWS LA English DT Review ID SINGLE-LAYER MOS2; MONOLAYER MOLYBDENUM-DISULFIDE; SCANNING-TUNNELING-MICROSCOPY; EFFICIENT HYDROGEN EVOLUTION; CHEMICALLY EXFOLIATED MOS2; ATOMICALLY THIN MOS2; ELECTRONIC-PROPERTIES; LITHIUM INTERCALATION; ULTRATHIN NANOSHEETS; COLLOIDAL SYNTHESIS AB Transition metal dichalcogenides (TMDs) represent a family of materials with versatile electronic, optical, and chemical properties. Most TMD bulk crystals are van der Waals solids with strong bonding within the plane but weak interlayer bonding. The individual layers can be readily isolated. Single layer TMDs possess intriguing properties that are ideal for both fundamental and technologically relevant research studies. We review the structure and phases of single and few layered TMDs. We also describe recent progress in phase engineering in TMDs. The ability to tune the chemistry by choosing a unique combination of transition metals and chalcogen atoms along with controlling their properties by phase engineering allows new functionalities to be realized with TMDs. C1 [Voiry, Damien; Chhowalla, Manish] Rutgers State Univ, Mat Sci & Engn, Piscataway, NJ 08854 USA. [Mohite, Aditya] Los Alamos Natl Lab, Mat Phys & Applicat Div, Los Alamos, NM 87545 USA. RP Chhowalla, M (reprint author), Rutgers State Univ, Mat Sci & Engn, 607 Taylor Rd, Piscataway, NJ 08854 USA. EM manish1@rci.rutgers.edu RI Voiry, Damien/G-3541-2016; OI Voiry, Damien/0000-0002-1664-2839; MOHITE, ADITYA/0000-0001-8865-409X NR 98 TC 67 Z9 67 U1 53 U2 238 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 0306-0012 EI 1460-4744 J9 CHEM SOC REV JI Chem. Soc. Rev. PY 2015 VL 44 IS 9 BP 2702 EP 2712 DI 10.1039/c5cs00151j PG 11 WC Chemistry, Multidisciplinary SC Chemistry GA CG9RX UT WOS:000353658000009 PM 25891172 ER PT S AU Muir, RD Pogranichniy, NR Muir, JL Sullivan, SZ Battaile, KP Mulichak, AM Toth, SJ Keefe, LJ Simpson, GJ AF Muir, Ryan D. Pogranichniy, Nicholas R. Muir, J. Lewis Sullivan, Shane Z. Battaile, Kevin P. Mulichak, Anne M. Toth, Scott J. Keefe, Lisa J. Simpson, Garth J. BE Bouman, CA Sauer, KD TI Spectral X-Ray Diffraction using a 6 Megapixel Photon Counting Array Detector SO COMPUTATIONAL IMAGING XIII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Computational Imaging XIII CY FEB 10-11, 2015 CL San Francisco, CA SP Soc Imaging Sci & Technol, SPIE ID RADIATION-DAMAGE; PROTEIN; CRYSTALLOGRAPHY AB Pixel-array array detectors allow single-photon counting to be performed on a massively parallel scale, with several million counting circuits and detectors in the array. Because the number of photoelectrons produced at the detector surface depends on the photon energy, these detectors offer the possibility of spectral imaging. In this work, a statistical model of the instrument response is used to calibrate the detector on a per-pixel basis. In turn, the calibrated sensor was used to perform separation of dual-energy diffraction measurements into two monochromatic images. Targeting applications include multi-wavelength diffraction to aid in protein structure determination and X-ray diffraction imaging. C1 [Muir, Ryan D.; Pogranichniy, Nicholas R.; Sullivan, Shane Z.; Toth, Scott J.; Keefe, Lisa J.; Simpson, Garth J.] Purdue Univ, Dept Chem, W Lafayette, IN 47906 USA. [Muir, J. Lewis; Battaile, Kevin P.; Mulichak, Anne M.] Argonne Natl Lab, Hauptman Woodward Med Res Inst, IMCA CAT, Argonne, IL 60439 USA. RP Muir, RD (reprint author), Purdue Univ, Dept Chem, 560 Oval Dr, W Lafayette, IN 47906 USA. OI Battaile, Kevin/0000-0003-0833-3259 FU NIGMS NIH HHS [R01 GM103401, R01 GM103910] NR 13 TC 0 Z9 0 U1 0 U2 3 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-1-62841-491-2 J9 PROC SPIE PY 2015 VL 9401 AR 940109 DI 10.1117/12.2079548 PG 5 WC Engineering, Electrical & Electronic; Optics; Imaging Science & Photographic Technology SC Engineering; Optics; Imaging Science & Photographic Technology GA BC5AJ UT WOS:000353126600007 PM 27041789 ER PT S AU Sreehari, S Venkatakrishnan, SV Drummy, LF Simmons, JP Bouman, CA AF Sreehari, Suhas Venkatakrishnan, S. V. Drummy, Lawrence F. Simmons, Jeffrey P. Bouman, Charles A. BE Bouman, CA Sauer, KD TI Advanced Prior Modeling for 3D Bright Field Electron Tomography SO COMPUTATIONAL IMAGING XIII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Computational Imaging XIII CY FEB 10-11, 2015 CL San Francisco, CA SP Soc Imaging Sci & Technol, SPIE DE Non-local means; plug-and-play; bright field; 3D tomography ID NONLOCAL-MEANS; RECONSTRUCTION; FRAMEWORK; ALGORITHM; IMAGES AB Many important imaging problems in material science involve reconstruction of images containing repetitive non-local structures. Model-based iterative reconstruction (MBIR) could in principle exploit such redundancies through the selection of a log prior probability term. However, in practice, determining such a log prior term that accounts for the similarity between distant structures in the image is quite challenging. Much progress has been made in the development of denoising algorithms like non-local means and BM3D, and these are known to successfully capture non-local redundancies in images. But the fact that these denoising operations are not explicitly formulated as cost functions makes it unclear as to how to incorporate them in the MBIR framework. In this paper, we formulate a solution to bright field electron tomography by augmenting the existing bright field MBIR method to incorporate any non-local denoising operator as a prior model. We accomplish this using a framework we call plug-and-play priors that decouples the log likelihood and the log prior probability terms in the MBIR cost function. We specifically use 3D non-local means (NLM) as the prior model in the plug-and-play framework, and showcase high quality tomographic reconstructions of a simulated aluminum spheres dataset, and two real datasets of aluminum spheres and ferritin structures. We observe that streak and smear artifacts are visibly suppressed, and that edges are preserved. Also, we report lower RMSE values compared to the conventional MBIR reconstruction using qGGMRF as the prior model. C1 [Sreehari, Suhas; Bouman, Charles A.] Purdue Univ, Sch ECE, W Lafayette, IN 47907 USA. [Venkatakrishnan, S. V.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Drummy, Lawrence F.; Simmons, Jeffrey P.] Air Force Res Lab, Dayton, OH USA. RP Sreehari, S (reprint author), Purdue Univ, Sch ECE, W Lafayette, IN 47907 USA. EM ssreehar@purdue.edu NR 26 TC 1 Z9 1 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 978-1-62841-491-2 J9 PROC SPIE PY 2015 VL 9401 AR 940108 DI 10.1117/12.2185603 PG 12 WC Engineering, Electrical & Electronic; Optics; Imaging Science & Photographic Technology SC Engineering; Optics; Imaging Science & Photographic Technology GA BC5AJ UT WOS:000353126600006 ER PT S AU Moen, EK Beier, HT Thompson, GL Armani, AM Ibey, BL AF Moen, Erick K. Beier, Hope T. Thompson, Gary L. Armani, Andrea M. Ibey, Bennett L. BE Ryan, TP TI Nonlinear Imaging of Lipid Membrane Alterations Elicited by Nanosecond Pulsed Electric Fields SO ENERGY-BASED TREATMENT OF TISSUE AND ASSESSMENT VIII SE Proceedings of SPIE LA English DT Proceedings Paper CT SPIE Conference on Energy-Based Treatment of Tissue and Assessment VIII CY FEB 08-09, 2015 CL San Francisco, CA SP SPIE ID ELECTROPORATION AB Second Harmonic Generation (SHG) imaging is a useful tool for examining the structure of interfaces between bulk materials. Recently, this technique was applied to detecting subtle perturbations in the structure of cellular membranes following nanosecond pulsed electric field (nsPEF) exposure. Monitoring the cell's outer membrane as it is exposed to nsPEF via SHG has demonstrated that nanoporation is likely the root cause for size-specific, increased cytoplasmic membrane permeabilization. It is theorized that the area of the membrane covered by these pores is tied to pulse intensity or duration. The extent of this effect along the cell's surface, however, has never been measured due to its temporal brevity and minute pore size. By enhancing the SHG technique developed and elucidated previously, we are able to obtain this information. Further, we vary the pulse width and amplitude of the applied stimulus to explore the mechanical changes of the membrane at various sites around the cell. By using this unique SHG imaging technique to directly visualize the change in order of phospholipids within the membrane, we are able to better understand the complex response of living cells to electric pulses. C1 [Moen, Erick K.; Armani, Andrea M.] Univ So Calif, Ming Hsieh Dept Elect Engn Electrophys, Los Angeles, CA 90095 USA. [Beier, Hope T.] JBSA Ft Sam Houston, Human Performance Wing 711, Air Force Res Lab,Opt Radiat Bioeffects Branch, Bioeffects Div,Human Effectiveness Directorate, San Antonio, TX USA. [Thompson, Gary L.] JBSA Ft Sam Houston, Oak Ridge Inst Sci & Educ, San Antonio, TX USA. [Ibey, Bennett L.] JBSA Ft Sam Houston, Human Performance Wing 711, Human Effectiveness Directorate,Air Force Res Lab, Radio Frequency Bioeffects Branch,Bioeffects Div, San Antonio, TX USA. RP Moen, EK (reprint author), Univ So Calif, Ming Hsieh Dept Elect Engn Electrophys, 920 Bloom Walk,SSC 502, Los Angeles, CA 90095 USA. NR 7 TC 0 Z9 0 U1 2 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 978-1-62841-416-5 J9 PROC SPIE PY 2015 VL 9326 AR 93260T DI 10.1117/12.2079452 PG 5 WC Engineering, Biomedical; Optics; Radiology, Nuclear Medicine & Medical Imaging SC Engineering; Optics; Radiology, Nuclear Medicine & Medical Imaging GA BC5SU UT WOS:000353555600027 ER PT J AU Vanston, CR Kearley, GJ Edwards, AJ Darwish, TA de Souza, NR Ramirez-Cuesta, AJ Gardiner, MG AF Vanston, C. R. Kearley, G. J. Edwards, A. J. Darwish, T. A. de Souza, N. R. Ramirez-Cuesta, A. J. Gardiner, M. G. TI The free-energy barrier to hydride transfer across a dipalladium complex SO FARADAY DISCUSSIONS LA English DT Article ID AUGMENTED-WAVE METHOD; MOLECULAR-DYNAMICS; NEUTRON-SCATTERING; PALLADIUM-HYDRIDE; HYDROGEN STORAGE; CLUSTER; COPOLYMERIZATION; REDUCTION; CATALYSIS; RELEVANT AB We use density-functional theory molecular dynamics (DFT-MD) simulations to determine the hydride transfer coordinate between palladium centres of the crystallographically observed terminal hydride locations, Pd-Pd-H, originally postulated for the solution dynamics of the complex bis-NHC dipalladium hydride [{(MesIm)(2)CH2}(2)Pd2H][PF6], and then calculate the free-energy along this coordinate. We estimate the transfer barrier-height to be about 20 kcal mol(-1) with a hydride transfer rate in the order of seconds at room temperature. We validate our DFT-MD modelling using inelastic neutron scattering which reveals anharmonicity of the hydride environment that is so pronounced that there is complete failure of the harmonic model for the hydride ligand. The simulations are extended to high temperature to bring the H-transfer to a rate that is accessible to the simulation technique. C1 [Vanston, C. R.; Gardiner, M. G.] Univ Tasmania, Sch Phys Sci Chem, Hobart, Tas, Australia. [Kearley, G. J.; Edwards, A. J.; Darwish, T. A.; de Souza, N. R.] Australian Nucl Sci & Technol Org, Bragg Inst, Kirrawee Dc, NSW 2232, Australia. [Ramirez-Cuesta, A. J.] Oak Ridge Natl Lab, Chem & Engn Div, Oak Ridge, TN 37831 USA. RP Gardiner, MG (reprint author), Univ Tasmania, Sch Phys Sci Chem, Private Bag 75, Hobart, Tas, Australia. EM Michael.Gardiner@utas.edu.au RI Ramirez-Cuesta, Timmy/A-4296-2010; OI Ramirez-Cuesta, Timmy/0000-0003-1231-0068; Gardiner, Michael/0000-0001-6373-4253 FU Access to Major Research Facilities Program (AMRFP); AINSE; University of Tasmania; Australian Research Council FX We would like to acknowledge beamtime on TOSCA at the ISIS facility, Oxford and the National Deuteration Facility, ANSTO for access via proposal NDF1196. Thanks to the Access to Major Research Facilities Program (AMRFP) for travel funding. Thanks to AINSE (for Research Awards and Postgraduate Research Award to CRV), the University of Tasmania (scholarship support for CRV) and the Australian Research Council for major project funding (Discovery Grant). NR 26 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 1359-6640 EI 1364-5498 J9 FARADAY DISCUSS JI Faraday Discuss. PY 2015 VL 177 BP 99 EP 109 DI 10.1039/c4fd00182f PG 11 WC Chemistry, Physical SC Chemistry GA CG1LO UT WOS:000353034300007 PM 25652724 ER PT J AU Marino, A Buron-Le Cointe, M Lorenc, M Toupet, L Henning, R DiChiara, AD Moffat, K Brefueld, N Collet, E AF Marino, A. Buron-Le Cointe, M. Lorenc, M. Toupet, L. Henning, R. DiChiara, A. D. Moffat, K. Brefueld, N. Collet, E. TI Out-of-equilibrium dynamics of photoexcited spin-state concentration waves SO FARADAY DISCUSSIONS LA English DT Article ID CROSSOVER COMPOUND; TRANSITION; COMPLEXES; SPECTROSCOPY; PHASE AB The spin crossover compound [(FeH2L2-Me)-H-II][PF6](2) presents a two-step phase transition. In the intermediate phase, a spin state concentration wave (SSCW) appears resulting from a symmetry breaking (cell doubling) associated with a long-range order of alternating high and low spin molecular states. By combining time-resolved optical and X-ray diffraction measurements on a single crystal, we study how such a system responds to femtosecond laser excitation and we follow in real time the erasing and rewriting of the SSCW. C1 [Marino, A.; Buron-Le Cointe, M.; Lorenc, M.; Toupet, L.; Collet, E.] Univ Rennes 1, CNRS, UMR 6251, Inst Phys Rennes, F-35042 Rennes, France. [Henning, R.; Moffat, K.] Univ Chicago, Ctr Adv Radiat Sources, Chicago, IL 60637 USA. [DiChiara, A. D.] Argonne Natl Lab, Argonne, IL 60439 USA. [Brefueld, N.] CEA CNRS, OMNT, F-38053 Grenoble, France. RP Buron-Le Cointe, M (reprint author), Univ Rennes 1, CNRS, UMR 6251, Inst Phys Rennes, F-35042 Rennes, France. EM marylise.buron@univ-rennes1.fr; eric.collet@univ-rennes1.fr RI Lorenc, Maciej/N-7594-2014; buron-le cointe, marylise/N-7592-2014; Collet, Eric/N-8816-2013 OI Collet, Eric/0000-0003-0810-7411 FU CNRS; Region Bretagne; Institut Universitaire de France, Rennes Metropole; ANR [ANR-13-BS04-0002]; European Regional Development Fund (FEDER); NIH [R24 GM111072]; University of Chicago through "France and Chicago Collaborating in the Sciences" (FACCTS) program; DOE Office of Science by Argonne National Laboratory [DE-AC02-06CH11357] FX This work was supported by the CNRS and Region Bretagne (PhD support of A.M.), the Institut Universitaire de France, Rennes Metropole, the ANR (ANR-13-BS04-0002) and the European Regional Development Fund (FEDER). BioCARS is funded by NIH grant R24 GM111072 to K.M. K.M. and E.C. thank the University of Chicago for funding through the "France and Chicago Collaborating in the Sciences" (FACCTS) program. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. NR 32 TC 6 Z9 6 U1 0 U2 11 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1359-6640 EI 1364-5498 J9 FARADAY DISCUSS JI Faraday Discuss. PY 2015 VL 177 BP 363 EP 379 DI 10.1039/c4fd00164h PG 17 WC Chemistry, Physical SC Chemistry GA CG1LO UT WOS:000353034300022 PM 25627455 ER PT J AU Hunt, AJ Matharu, AS King, AH Clark, JH AF Hunt, Andrew J. Matharu, Avtar S. King, Alexander H. Clark, James H. TI The importance of elemental sustainability and critical element recovery SO GREEN CHEMISTRY LA English DT Editorial Material C1 [Hunt, Andrew J.; Matharu, Avtar S.; Clark, James H.] Univ York, Green Chem Ctr Excellence, Dept Chem, York YO10 5DD, N Yorkshire, England. [King, Alexander H.] USDA, Ames Lab, Crit Mat Inst, Ames, IA 50011 USA. RP Hunt, AJ (reprint author), Univ York, Green Chem Ctr Excellence, Dept Chem, York YO10 5DD, N Yorkshire, England. EM andrew.hunt@york.ac.uk RI King, Alexander/P-6497-2015; OI King, Alexander/0000-0001-7101-6585; Hunt, Andrew/0000-0003-3983-8313 NR 5 TC 8 Z9 8 U1 4 U2 27 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9262 EI 1463-9270 J9 GREEN CHEM JI Green Chem. PY 2015 VL 17 IS 4 BP 1949 EP 1950 DI 10.1039/c5gc90019k PG 2 WC Chemistry, Multidisciplinary; GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY SC Chemistry; Science & Technology - Other Topics GA CF7GL UT WOS:000352724200001 ER PT J AU Mante, OD Rodriguez, JA Senanayake, SD Babu, SP AF Mante, Ofei D. Rodriguez, Jose A. Senanayake, Sanjaya D. Babu, Suresh P. TI Catalytic conversion of biomass pyrolysis vapors into hydrocarbon fuel precursors SO GREEN CHEMISTRY LA English DT Article ID C COUPLING REACTIONS; ACETIC-ACID; PHASE KETONIZATION; CARBOXYLIC-ACIDS; OXIDES; CERIA; OIL; KETONES AB We report on a new pyrolytic pathway for biomass conversion to hydrocarbon fuel precursors. The process entails the conversion of multifunctional oxygenates generated from biomass pyrolysis over a metal oxide catalyst into ketonic-rich monofunctional molecules suitable for making hydrocarbon fuel components for gasoline, diesel, and jet fuel. A number of catalysts were explored, for example, anatase TiO2 nanorods, CeOx-TiO2 mixed oxides, pure CeO2, ZrO2, and MgO. Under pyrolysis conditions, ceria-based catalysts were effective in the conversion of hydroxy-carbonyls, anhydrosugars, and carboxylic acids into acetone, 2-butanone, pentanones, C6/C7 ketones, cyclopentanone, and 2-cyclopentenones. The highest carbon yield (23.5%) of ketonic precursors was achieved on the pure CeO2. C1 [Mante, Ofei D.; Babu, Suresh P.] Brookhaven Natl Lab, Sustainable Energy Technol Dept, Upton, NY 11973 USA. [Rodriguez, Jose A.; Senanayake, Sanjaya D.] Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA. RP Mante, OD (reprint author), Brookhaven Natl Lab, Sustainable Energy Technol Dept, Upton, NY 11973 USA. EM nmante@bnl.gov RI Mante, Ofei/E-8513-2014; Senanayake, Sanjaya/D-4769-2009 OI Mante, Ofei/0000-0002-0960-2943; Senanayake, Sanjaya/0000-0003-3991-4232 FU Brookhaven National Laboratory Internal Funding, LDRD project [19086] FX The authors acknowledge financial support from Brookhaven National Laboratory Internal Funding, LDRD project #19086. Dr Weiqiang Han (formerly of the Center for Functional Nanomaterials at BNL) is acknowledged for the synthesis of the anatase TiO2 nanorods. We would also like to thank Dr Shankhamala Kundu for catalyst impregnation efforts. NR 27 TC 2 Z9 2 U1 7 U2 34 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9262 EI 1463-9270 J9 GREEN CHEM JI Green Chem. PY 2015 VL 17 IS 4 BP 2362 EP 2368 DI 10.1039/c4gc02238f PG 7 WC Chemistry, Multidisciplinary; GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY SC Chemistry; Science & Technology - Other Topics GA CF7GL UT WOS:000352724200040 ER PT J AU Neupane, S Adhikari, S Wang, Z Ragauskas, AJ Pu, Y AF Neupane, S. Adhikari, S. Wang, Z. Ragauskas, A. J. Pu, Y. TI Effect of torrefaction on biomass structure and hydrocarbon production from fast pyrolysis SO GREEN CHEMISTRY LA English DT Article ID CATALYTIC FAST PYROLYSIS; BIO-OIL; LOBLOLLY-PINE; LIGNIN; CELLULOSE; WOOD; LEVOGLUCOSAN; PRETREATMENT; TEMPERATURE; CHEMISTRY AB Torrefaction has been shown to improve the chemical composition of bio-oils produced from fast pyrolysis by lowering its oxygen content and enhancing the aromatic yield. A Py-GC/MS study was employed to investigate the effect of torrefaction temperatures (225, 250 and 275 degrees C) and residence times (15, 30 and 45 min) on product distribution from non-catalytic and H(+)ZSM-5 catalyzed pyrolysis of pinewood. During torrefaction, structural transformations in biomass constitutive polymers: hemicellulose, cellulose and lignin took place, which were evaluated using component analysis, solid state CP/MAS C-13 NMR and XRD techniques. Torrefaction caused deacetylation and decomposition of hemicellulose, cleavage of aryl ether linkages and demethoxylation of lignin, degradation of cellulose and an overall increase in aromaticity of biomass, all of which affected the product yield from pyrolysis of torrefied biomass. For non-catalytic pyrolysis, selectivity of phenolic compounds increased with an increase in torrefaction severity while that of furan compounds decreased. In the case of catalytic pyrolysis, the sample torrefied at 225 degrees C-30 min and 250 degrees C-15 min resulted in a significant increase in aromatic hydrocarbon (HC) and also total carbon yield (approx. 1.6 times higher) as compared to catalytic pyrolysis of non-torrefied pine. Cleavage of aryl ether linkages and demethoxylation in lignin due to torrefaction caused increased yield of phenolic compounds, which in the presence of a catalyst were dehydrated to form aromatic HC. C1 [Neupane, S.; Adhikari, S.; Wang, Z.] Auburn Univ, Biosyst Engn Dept, Auburn, AL 36849 USA. [Ragauskas, A. J.] Univ Tennessee, Dept Chem & Biomol Engn, Knoxville, TN 37996 USA. [Pu, Y.] Oak Ridge Natl Lab, Biosci Div, Oak Ridge, TN 37831 USA. RP Neupane, S (reprint author), Auburn Univ, Biosyst Engn Dept, Auburn, AL 36849 USA. EM sushil.adhikari@auburn.edu RI Pu, Yunqiao/H-3206-2016 OI Pu, Yunqiao/0000-0003-2554-1447 FU National Science Foundation [NSF-CBET-1333372] FX The authors acknowledge the National Science Foundation (NSF-CBET-1333372) for funding this study. Also, the authors would like to thank Mr Chad Carter for preparing torrefied biomass samples for this study. However, only the authors are responsible for any remaining errors in this paper. NR 49 TC 19 Z9 19 U1 6 U2 58 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9262 EI 1463-9270 J9 GREEN CHEM JI Green Chem. PY 2015 VL 17 IS 4 BP 2406 EP 2417 DI 10.1039/c4gc02383h PG 12 WC Chemistry, Multidisciplinary; GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY SC Chemistry; Science & Technology - Other Topics GA CF7GL UT WOS:000352724200046 ER PT J AU Schwaiger, N Elliott, DC Ritzberger, J Wang, H Pucher, P Siebenhofer, M AF Schwaiger, N. Elliott, D. C. Ritzberger, J. Wang, H. Pucher, P. Siebenhofer, M. TI Hydrocarbon liquid production via the bioCRACK process and catalytic hydroprocessing of the product oil SO GREEN CHEMISTRY LA English DT Article ID BIO-OIL; BIOCHAR LIQUEFACTION; PHASE PYROLYSIS AB Continuous hydroprocessing of liquid phase pyrolysis Bio-oil, provided by BDI-BioEnergy International bioCRACK pilot plant at OMV Refinery in Schwechat/Vienna Austria was investigated. These hydroprocessing tests showed promising results using catalytic hydroprocessing strategies developed for unfractionated Bio-oil. A sulfided base metal catalyst (CoMo on Al2O3) was evaluated. The bed of catalyst was operated at 400 degrees C in a continuous-flow reactor at a pressure of 12.1 MPa with flowing hydrogen. The condensed liquid products were analyzed and found that the hydrocarbon liquid was significantly hydrotreated so that nitrogen and sulfur were below the level of detection (<0.05), while the residual oxygen ranged from 0.7 to 1.2%. The density of the products varied from 0.71 g mL(-1) up to 0.79 g mL(-1) with a correlated change of the hydrogen to carbon atomic ratio from 2.1 down to 1.9. The product quality remained high throughout the extended tests suggesting minimal loss of catalyst activity through the test. These tests provided the data needed to assess the quality of liquid fuel products obtained from the bioCRACK process as well as the activity of the catalyst for comparison with products obtained from hydrotreated fast pyrolysis Bio-oils from fluidized-bed operation. C1 [Schwaiger, N.; Siebenhofer, M.] Graz Univ Technol, Cent Lab Biobased Prod, NAWI Graz, Inst Chem Engn & Environm Technol, A-8010 Graz, Austria. [Elliott, D. C.; Wang, H.] Pacific NW Natl Lab, Richland, WA 99352 USA. [Schwaiger, N.; Ritzberger, J.; Pucher, P.] BDI BioEnergy Int AG, A-8074 Graz, Austria. RP Schwaiger, N (reprint author), Graz Univ Technol, Cent Lab Biobased Prod, NAWI Graz, Inst Chem Engn & Environm Technol, Inffeldgasse 25-C, A-8010 Graz, Austria. EM nikolaus.schwaiger@tugraz.at FU U.S. Department of Energy, Bio-oil Stabilization and Commoditization FOA at the Pacific Northwest National Laboratory [0686, DE-AC05-76RL01830]; BDI-BioEnergy International AG FX This research work was supported by BDI-BioEnergy International AG under Work-For-Others contract. The preparation of the publication was performed with support from the U.S. Department of Energy as part of the Bio-oil Stabilization and Commoditization FOA #0686 under Contract No. DE-AC05-76RL01830 at the Pacific Northwest National Laboratory. The authors gratefully acknowledge the support of the Bioenergy Technologies Office and program manager Prasad Gupta. Suh-Jane Lee and Asanga Padmaperuma are acknowledged for their participation in the operations of the minihydrotreater. NR 19 TC 6 Z9 6 U1 1 U2 19 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9262 EI 1463-9270 J9 GREEN CHEM JI Green Chem. PY 2015 VL 17 IS 4 BP 2487 EP 2494 DI 10.1039/c4gc02344g PG 8 WC Chemistry, Multidisciplinary; GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY SC Chemistry; Science & Technology - Other Topics GA CF7GL UT WOS:000352724200055 ER PT S AU Oktem, R Dafflon, B Peterson, JE Hubbard, SS AF Oektem, Rusen Dafflon, Baptiste Peterson, John E. Hubbard, Susan S. BE Lam, EY Niel, KS TI Monitoring Arctic Landscape Variation by Pole and Kite Mounted Cameras SO IMAGE PROCESSING: MACHINE VISION APPLICATIONS VIII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Image Processing - Machine Vision Applications VIII CY FEB 10-11, 2015 CL San Francisco, CA SP Soc Imaging Sci & Technol, SPIE DE vegetation monitoring; landscape monitoring; segmentation; feature extraction AB Optic surveillance is an important part of monitoring environmental changes in various ecological settings. Although remote sensing provides extensive data, its resolution is yet not sufficient for scientific research focusing on small spatial scale landscape variations. We are interested in exploiting high resolution image data to observe and investigate the landscape variations at a small spatial scale arctic corridor in Barrow, AK, as part of the DOE Next-Generation Ecosystem Experiments (NGEE-Arctic). A 35 m transect is continuously imaged by two separate pole mounted consumer grade stationary cameras, one capturing in NIR and the other capturing in visible range, starting from June to August in 2014. Surface and subsurface features along this 35 m transect are also sampled by electrical resistivity tomography (ERT), temperature loggers and water content reflectometers. We track the behavioral change along this transect by collecting samples from the pole images and look for a relation between the image features and electrical conductivity. Results show that the correlation coefficient between inferred vegetation indices and soil electrical resistivity (closely related to water content) increased during the growing season, reaching a correlation of 0.89 at the peak of the vegetation. To extrapolate such results to a larger scale, we use a high resolution RGB map of a 500x40 m corridor at this site, which is occasionally obtained using a low-altitude kite mounted consumer grade (RGB) camera. We introduce a segmentation algorithm that operates on the mosaic generated from the kite images to classify the landscape features of the corridor. C1 [Oektem, Rusen] Univ Calif Berkeley, Dept Earth & Planetary Sci, Berkeley, CA 94720 USA. [Dafflon, Baptiste; Peterson, John E.; Hubbard, Susan S.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. RP Oktem, R (reprint author), Univ Calif Berkeley, Dept Earth & Planetary Sci, 307 Mc Cone Hall, Berkeley, CA 94720 USA. EM roktem@lbl.gov RI Dafflon, Baptiste/G-2441-2015; Hubbard, Susan/E-9508-2010 NR 6 TC 0 Z9 0 U1 2 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 978-1-62841-495-0 J9 PROC SPIE PY 2015 VL 9405 AR 940505 PG 7 WC Computer Science, Artificial Intelligence; Optics; Imaging Science & Photographic Technology SC Computer Science; Optics; Imaging Science & Photographic Technology GA BC5JO UT WOS:000353328200003 ER PT S AU Ruggiero, C Ross, A Porter, R AF Ruggiero, Christy Ross, Amy Porter, Reid BE Lam, EY Niel, KS TI Segmentation and Learning in the Quantitative Analysis of Microscopy Images SO Image Processing: Machine Vision Applications VIII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Image Processing - Machine Vision Applications VIII CY FEB 10-11, 2015 CL San Francisco, CA SP Soc Imaging Sci & Technol, SPIE DE segmentation; supervised segmentation; image quantification; microscopy; material science ID INTERACTIVE SEGMENTATION; SCIENCE AB In material science and bio-medical domains the quantity and quality of microscopy images is rapidly increasing and there is a great need to automatically detect, delineate and quantify particles, grains, cells, neurons and other functional " objects" within these images. These are challenging problems for image processing because of the variability in object appearance that inevitably arises in real world image acquisition and analysis. One of the most promising (and practical) ways to address these challenges is interactive image segmentation. These algorithms are designed to incorporate input from a human operator to tailor the segmentation method to the image at hand. Interactive image segmentation is now a key tool in a wide range of applications in microscopy and elsewhere. Historically, interactive image segmentation algorithms have tailored segmentation on an image-by-image basis, and information derived from operator input is not transferred between images. But recently there has been increasing interest to use machine learning in segmentation to provide interactive tools that accumulate and learn from the operator input over longer periods of time. These new learning algorithms reduce the need for operator input over time, and can potentially provide a more dynamic balance between customization and automation for different applications. This paper reviews the state of the art in this area, provides a unified view of these algorithms, and compares the segmentation performance of various design choices. C1 [Ruggiero, Christy] Los Alamos Natl Lab, Nucl Engn & Nonproliferat, Los Alamos, NM 87545 USA. [Ross, Amy] Los Alamos Natl Lab, Nucl Mat Sci, Los Alamos, NM 87545 USA. [Porter, Reid] Los Alamos Natl Lab, Intelligence & Space Res, Los Alamos, NM 87545 USA. RP Ruggiero, C (reprint author), Los Alamos Natl Lab, Nucl Engn & Nonproliferat, POB 1663, Los Alamos, NM 87545 USA. EM rporter@lanl.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 978-1-62841-495-0 J9 PROC SPIE PY 2015 VL 9405 AR 94050L PG 9 WC Computer Science, Artificial Intelligence; Optics; Imaging Science & Photographic Technology SC Computer Science; Optics; Imaging Science & Photographic Technology GA BC5JO UT WOS:000353328200017 ER PT J AU Garanin, SF Kuznetsov, SD Reinovsky, RE AF Garanin, S. F. Kuznetsov, S. D. Reinovsky, R. E. TI Feasibility of warm dense matter generation using aluminum and copper foil electric explosion under the PHELIX facility current drive SO JOURNAL OF APPLIED MECHANICS AND TECHNICAL PHYSICS LA English DT Article DE warm dense matter; equation of state; electric explosion; Joule heating AB This paper investigates the feasibility of using the PHELIX facility for generation of warm dense matter (WDM), i.e., substance at densities of the order of 0.01-1.00 of the solid matter density and a temperature of 1-10 eV, by electric explosion of a thin cylindrical metal foil enclosed in an insulator. It has been shown this system can be used to produce a significant volume of uniform WDM with a density of 0.1-1.0 g/cm(3) and a temperature of 3-4 eV, sufficient for electrical measurements. A method of determining WDM parameters based on electrical measurements and foil boundary velocimetry is described. C1 [Garanin, S. F.; Kuznetsov, S. D.] Russian Federat Nucl Ctr, Inst Expt Phys VNIIEF, Sarov 607188, Russia. [Reinovsky, R. E.] Los Alamos Natl Lab, Los Alamos, NM USA. RP Garanin, SF (reprint author), Russian Federat Nucl Ctr, Inst Expt Phys VNIIEF, Sarov 607188, Russia. EM sfgar@vniief.ru; S.D.Kuznetsov@vniief.ru; bobr@lanl.gov NR 13 TC 0 Z9 0 U1 0 U2 3 PU MAIK NAUKA/INTERPERIODICA/SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013-1578 USA SN 0021-8944 EI 1573-8620 J9 J APPL MECH TECH PH+ JI J. Appl. Mech. Tech. Phys. PD JAN PY 2015 VL 56 IS 1 BP 10 EP 15 DI 10.1134/S0021894415010022 PG 6 WC Mechanics; Physics, Applied SC Mechanics; Physics GA CF9QB UT WOS:000352899300002 ER PT J AU Yin, WJ Yang, JH Kang, J Yan, YF Wei, SH AF Yin, Wan-Jian Yang, Ji-Hui Kang, Joongoo Yan, Yanfa Wei, Su-Huai TI Halide perovskite materials for solar cells: a theoretical review SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Review ID HOLE-CONDUCTOR-FREE; METHYLAMMONIUM LEAD IODIDE; QUASI-RANDOM STRUCTURES; ELECTRONIC-PROPERTIES; HIGH-EFFICIENCY; 1ST-PRINCIPLES CALCULATION; PHOTOVOLTAIC MATERIALS; SEQUENTIAL DEPOSITION; STRUCTURAL-PROPERTIES; BROMIDE PEROVSKITE AB Halide perovskites have recently emerged as promising materials for low-cost, high-efficiency solar cells. The efficiency of perovskite-based solar cells has increased rapidly, from 3.8% in 2009 to 19.3% in 2014, by using the all-solid-state thin-film architecture and engineering cell structures with mixed-halide perovskites. The emergence of perovskite solar cells revolutionized the field not only because of their rapidly increased efficiency, but also flexibility in material growth and architecture. The superior performance of the perovskite solar cells suggested that perovskite materials possess intrinsically unique properties. In this review, we summarize recent theoretical investigations into the structural, electrical, and optical properties of halide perovskite materials in relation to their applications in solar cells. We also discuss some current challenges of using perovskites in solar cells, along with possible theoretical solutions. C1 [Yin, Wan-Jian; Yang, Ji-Hui; Kang, Joongoo; Wei, Su-Huai] Natl Renewable Energy Lab, Golden, CO 80401 USA. [Yin, Wan-Jian; Yan, Yanfa] Univ Toledo, Dept Phys & Astron, Toledo, OH 43606 USA. RP Yin, WJ (reprint author), Natl Renewable Energy Lab, Golden, CO 80401 USA. EM wan-jian.yin@nrel.gov; suhuai.wei@nrel.gov RI Yin, Wanjian/F-6738-2013 FU U.S. Department of Energy [DE-AC36-08GO28308]; National Renewable Energy Laboratory; DOE Office of Energy Efficiency and Renewable Energy; Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]; Ohio Research Scholar Program FX This research was funded by the U.S. Department of Energy under Grant no. DE-AC36-08GO28308 with the National Renewable Energy Laboratory. Funding for the work was provided by the DOE Office of Energy Efficiency and Renewable Energy. This work used the NREL Peregrine Supercomputer, the Ohio Supercomputer Center and 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. Y.Y. acknowledges the support of the Ohio Research Scholar Program. NR 138 TC 171 Z9 171 U1 106 U2 559 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7488 EI 2050-7496 J9 J MATER CHEM A JI J. Mater. Chem. A PY 2015 VL 3 IS 17 BP 8926 EP 8942 DI 10.1039/c4ta05033a PG 17 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA CG6OF UT WOS:000353420800002 ER PT J AU Zhao, YX Zhu, K AF Zhao, Yixin Zhu, Kai TI Three-step sequential solution deposition of PbI2-free CH3NH3PbI3 perovskite SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID ORGANOMETAL HALIDE PEROVSKITES; SOLUTION-PROCESSED PEROVSKITE; SENSITIZED SOLAR-CELL; CHARGE-TRANSPORT; EFFICIENT; TIO2; RECOMBINATION; PHOTOVOLTAICS AB We demonstrate a three-step sequential solution process to prepare PbI2-free CH3NH3PbI3 perovskite films. In this three-step method, a thermally unstable stoichiometric PbI2 center dot CH3NH3Cl precursor film is first deposited on the mesoporous TiO2 substrate, followed by thermal decomposition to form PbI2, which is finally converted into CH3NH3PbI3 by dipping in a regular isopropanol solution of CH3NH3I at room temperature. In comparison to the two-step approach using similar processing conditions, the three-step method enables the formation of the PbI2 film through the thermal decomposition of the PbI2 center dot CH3NH3Cl precursor film. This facilitates a rapid conversion of PbI2 to CH3NH3PbI3 without any traceable residue PbI2 in the final conversion step, leading to an improved device performance. C1 [Zhao, Yixin] Shanghai Jiao Tong Univ, Sch Environm Sci & Engn, Shanghai 200240, Peoples R China. [Zhu, Kai] Natl Renewable Energy Lab, Chem & Mat Sci Ctr, Golden, CO 80401 USA. RP Zhao, YX (reprint author), Shanghai Jiao Tong Univ, Sch Environm Sci & Engn, 800 Dongchuan Rd, Shanghai 200240, Peoples R China. EM yixin.zhao@sjtu.edu.cn; kai.zhu@nrel.gov RI Zhao, Yixin/D-2949-2012 FU NSFC [51372151, 21303103]; U.S. Department of Energy/National Renewable Energy Laboratory's Laboratory Directed Research and Development (LDRD) program [DE-AC36-08GO28308] FX YZ is thankful for the support of the NSFC (Grant 51372151 and 21303103). KZ acknowledges the support by the U.S. Department of Energy/National Renewable Energy Laboratory's Laboratory Directed Research and Development (LDRD) program under Contract no. DE-AC36-08GO28308. NR 30 TC 30 Z9 32 U1 9 U2 70 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7488 EI 2050-7496 J9 J MATER CHEM A JI J. Mater. Chem. A PY 2015 VL 3 IS 17 BP 9086 EP 9091 DI 10.1039/c4ta05384b PG 6 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA CG6OF UT WOS:000353420800017 ER PT J AU Zhou, YY Yang, MJ Vasiliev, AL Garces, HF Zhao, YX Wang, D Pang, SP Zhu, K Padture, NP AF Zhou, Yuanyuan Yang, Mengjin Vasiliev, Alexander L. Garces, Hector F. Zhao, Yixin Wang, Dong Pang, Shuping Zhu, Kai Padture, Nitin P. TI Growth control of compact CH3NH3PbI3 thin films via enhanced solid-state precursor reaction for efficient planar perovskite solar cells SO Journal of Materials Chemistry A LA English DT Article ID VAPOR-DEPOSITION; HOLE-CONDUCTOR; HETEROJUNCTION; IODIDE; CHEMISTRY; LENGTHS; LIGHT AB CH3NH3PbI3 (MAPbI(3)) perovskite thin films that are solution-processed using either a one-step or two-step conventional method typically contain a significant number of defects (voids, pinholes) or PbI2 impurities, which have a detrimental effect on the performance of planar perovskite solar cells (PSCs) fabricated using those films. To overcome this issue, we show that enhancement of the solid-state reaction between inorganic-organic precursors is an effective route for the growth of compact, phase-pure MAPbI(3) perovskite thin films with no voids or pinholes. To ensure uniform solid-state conversion (MAI + PbI2 -> MAPbI(3)) across the entire film thickness, a new successive spin coating/annealing (SSCA) process is used, where MAI is repeatedly infiltrated into a nanoporous PbI2 film, followed by thermal annealing. The mechanisms involved in the SSCA process are elucidated by monitoring the evolution of the phases during the reaction. Owing to these desirable characteristics (high-purity, full-coverage, enhanced smoothness and compactness) of the SSCA MAPbI(3) films, planar PSCs based on these perovskite thin films delivered a maximum power conversion efficiency (PCE) close to 15%. Furthermore, PSCs fabricated using partially converted nanoporous PbI2 thin films delivered a surprising PCE approaching 10%, suggesting continuous MAPbI(3) phase formation throughout the entire film at each spin coating/annealing process. The advantages gained from enhancing the solid-state precursor reactions allow better control of the growth of the perovskite making the SSCA process more robust. C1 [Zhou, Yuanyuan; Vasiliev, Alexander L.; Garces, Hector F.; Padture, Nitin P.] Brown Univ, Sch Engn, Providence, RI 02912 USA. [Yang, Mengjin; Zhu, Kai] Natl Renewable Energy Lab, Chem & Mat Sci Ctr, Golden, CO 80401 USA. [Zhao, Yixin] Shanghai Jiao Tong Univ, Sch Environm Sci & Engn, Shanghai 200240, Peoples R China. [Wang, Dong; Pang, Shuping] Chinese Acad Sci, Qingdao Inst Bioenergy & Bioproc Technol, Qingdao 266101, Peoples R China. RP Padture, NP (reprint author), Brown Univ, Sch Engn, Providence, RI 02912 USA. EM nitin_padture@brown.edu RI Zhao, Yixin/D-2949-2012; Zhou, Yuanyuan/G-2173-2011; Vasiliev, Alexander/E-9855-2014; Padture, Nitin/A-9746-2009 OI Zhou, Yuanyuan/0000-0002-8364-4295; Vasiliev, Alexander/0000-0001-7884-4180; Padture, Nitin/0000-0001-6622-8559 FU National Science Foundation [DMR-1305913]; Brown University Graduate School; U.S. Department of Energy [DE-AC36-08-GO28308]; U.S. Department of Energy (DOE) SunShot Initiative [DE-FOA-0000990] FX This study was supported by a grant from the National Science Foundation (Grant no. DMR-1305913) and the Brown University Graduate School, and the work at the National Renewable Energy Laboratory was supported by the U.S. Department of Energy under Contract no. DE-AC36-08-GO28308. M.Y. and K.Z. acknowledge the support by the U.S. Department of Energy (DOE) SunShot Initiative under the Next Generation Photovoltaics 3 program (DE-FOA-0000990). The authors' thank Prof. S. Kim, Mr P. Liu, Prof. D. Pacifici, and Mr M. Strauss of Brown University for the experimental assistance and fruitful discussions. NR 37 TC 39 Z9 40 U1 23 U2 124 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7488 EI 2050-7496 J9 J MATER CHEM A JI J. Mater. Chem. A PY 2015 VL 3 IS 17 BP 9249 EP 9256 DI 10.1039/c4ta07036d PG 8 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA CG6OF UT WOS:000353420800042 ER PT J AU Manbeck, GF Fujita, E AF Manbeck, Gerald F. Fujita, Etsuko TI A review of iron and cobalt porphyrins, phthalocyanines and related complexes for electrochemical and photochemical reduction of carbon dioxide SO JOURNAL OF PORPHYRINS AND PHTHALOCYANINES LA English DT Review DE CO2 reduction; porphyrin; phthalocyanine; cobalt; iron ID GAS-DIFFUSION ELECTRODES; ELECTROCATALYTIC CO2 REDUCTION; METAL PHTHALOCYANINES; GLASSY-CARBON; MOLECULAR CATALYSTS; HOMOGENEOUS CATALYSIS; GRAPHITE ELECTRODE; FUEL-CELLS; ELECTROREDUCTION; TETRAPHENYLPORPHYRIN AB This review summarizes research on the electrochemical and photochemical reduction of CO2 using a variety of iron and cobalt porphyrins, phthalocyanines and related complexes. Metalloporphyrins and metallophthalocyanines are visible light absorbers with extremely large extinction coefficients. However, yields of photochemically-generated active catalysts for CO2 reduction are typically low owing to the requirement of a second photoinduced electron. This requirement is not relevant to the case of electrochemical CO2 reduction. Recent progress on efficient and stable electrochemical systems includes the use of FeTPP catalysts that have prepositioned phenyl OH groups in their second coordination spheres. This has led to remarkable progress in carrying out coupled proton-electron transfer reactions for CO2 reduction. Such ground-breaking research has to be continued in order to produce renewable fuels in an economically feasible manner. C1 [Manbeck, Gerald F.; Fujita, Etsuko] Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA. RP Manbeck, GF (reprint author), Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA. EM gmanbeck@bnl.gov; fujita@bnl.gov FU U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-98CH10886] FX We thank Drs. James T. Muckerman and David C. Grills for careful reading of this manuscript. The work at Brookhaven National Laboratory was carried out under contract DE-AC02-98CH10886 with the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences. NR 84 TC 17 Z9 17 U1 50 U2 210 PU WORLD SCI PUBL CO INC PI HACKENSACK PA 27 WARREN ST, STE 401-402, HACKENSACK, NJ 07601 USA SN 1088-4246 EI 1099-1409 J9 J PORPHYR PHTHALOCYA JI J. Porphyr. Phthalocyanines PD JAN-MAR PY 2015 VL 19 IS 1-3 BP 45 EP 64 DI 10.1142/S1088424615300013 PG 20 WC Chemistry, Multidisciplinary SC Chemistry GA CF6CK UT WOS:000352644100006 ER PT J AU Eroglu, D Zavadil, KR Gallagher, KG AF Eroglu, Damla Zavadil, Kevin R. Gallagher, Kevin G. TI Critical Link between Materials Chemistry and Cell-Level Design for High Energy Density and Low Cost Lithium-Sulfur Transportation Battery SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID S BATTERIES; POLYSULFIDE SHUTTLE; CARBON NANOFIBERS; ELECTROLYTE; PERFORMANCE; CAPACITY; CATHODE; SPECTROSCOPY; STABILITY; LIFE AB A materials-to-system analysis for the lithium-sulfur (Li-S) electric vehicle battery is presented that identifies the key electrode and cell design considerations from reports of materials chemistry. The resulting systems-level energy density, specific energy and battery price as a function of these parameters is projected. Excess lithium metal amount at the anode and useable specific capacity, electrolyte volume fraction, sulfur to carbon ratio and reaction kinetics at the cathode are all shown to be critical for the high energy density and low cost requirements. Electrode loading is determined as a key parameter to relate the battery price for useable energy to the investigated design considerations. The presented analysis proposes that electrode loadings higher than 8 mAh/cm(2) (similar to 7 mg S/cm(2)) are necessary for Li-S systems to exhibit the high energy density and low cost required for transportation applications. Stabilizing the interface of lithium metal at the required current densities and areal capacities while simultaneously maintaining cell capacity with high sulfur loading in an electrolyte starved cathode are identified as the key barriers for ongoing research and development efforts to address. (C) The Author(s) 2015. All rights reserved. C1 [Eroglu, Damla; Gallagher, Kevin G.] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. [Zavadil, Kevin R.] Sandia Natl Labs, Albuquerque, NM 87185 USA. EM damlaeroglu@gmail.com FU Joint Center for Energy Storage Research, an Energy Innovation Hub - U.S. Department of Energy, Office of Science, Basic Energy Sciences; U.S. Department of Energy Office of Science laboratory [DE-AC02-06CH11357] FX This work was supported as part of the Joint Center for Energy Storage Research, an Energy Innovation Hub funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences. 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. NR 49 TC 22 Z9 22 U1 16 U2 53 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 EI 1945-7111 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2015 VL 162 IS 6 BP A982 EP A990 DI 10.1149/2.0611506jes PG 9 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA CG1BZ UT WOS:000353009300028 ER PT J AU Higa, K Srinivasan, V AF Higa, Kenneth Srinivasan, Venkat TI Stress and Strain in Silicon Electrode Models SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID LITHIUM-ION BATTERIES; CARBON-COATED SI; NEGATIVE ELECTRODES; ANODE MATERIAL; FRACTURE; INSERTION; LITHIATION; PARTICLES; NANOWIRES; BINDER AB While the high capacity of silicon makes it an attractive negative electrode for Li-ion batteries, the associated large volume change results in fracture and capacity fade. Composite electrodes incorporating silicon have additional complexity, as active material is attached to surrounding material which must likewise experience significant volume change. In this paper, a finite-deformation model is used to explore, for the first time, mechanical interactions between a silicon particle undergoing lithium insertion, and attached binder material. Simulations employ an axisymmetric model system in which solutions vary in two spatial directions and shear stresses develop at interfaces between materials. The mechanical response of the amorphous active material is dependent on lithium concentration, and an equation of state incorporating reported volume expansion data is used. Simulations explore the influence of active material size and binder stiffness, and suggest delamination as an additional mode of material damage. Computed strain energies and von Mises equivalent stresses are in physically-relevant ranges, comparable to reported yield stresses and adhesion energies, and predicted trends are largely consistent with reported experimental results. It is hoped that insights from this work will support the design of more robust silicon composite electrodes. (C) The Author(s) 2015. Published by ECS. This is an open access article distributed under the terms of the Creative Commons Attribution 4.0 License (CC BY, http://creativecommons.orylicenses/by/4.0/), which permits unrestricted reuse of the work in any medium, provided the original work is properly cited. All rights reserved. C1 [Higa, Kenneth; Srinivasan, Venkat] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Higa, K (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. EM KHiga@lbl.gov FU Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the U.S. Department of Energy under the Batteries for Advanced Transportation Technologies (BATT) Program [DE-AC02-05CH11231] FX This work was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231 under the Batteries for Advanced Transportation Technologies (BATT) Program. NR 41 TC 11 Z9 11 U1 10 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 2015 VL 162 IS 6 BP A1111 EP A1122 DI 10.1149/2.0091507jes PG 12 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA CG1BZ UT WOS:000353009300044 ER PT J AU Martin, MA Chen, CF Mukherjee, PP Pannala, S Dietiker, JF Turner, JA Ranjan, D AF Martin, Michael A. Chen, Chien-Fan Mukherjee, Partha P. Pannala, Sreekanth Dietiker, Jean-Francois Turner, John A. Ranjan, Devesh TI Morphological Influence in Lithium-Ion Battery 3D Electrode Architectures SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID FINITE-ELEMENT-ANALYSIS; RECHARGEABLE BATTERIES; FRACTAL ELECTRODES; ENERGY-STORAGE; INSERTION CELL; MICROBATTERIES; MODEL; ELECTROCHEMISTRY; FABRICATION; RELAXATION AB The performance of lithium-ion batteries is limited by suboptimal energy density and power capability. A feasible approach is designing 3D electrode architectures where lithium ion transport in the electrolyte and active material can be optimized for improving the energy/power density. In this study, the influence of active material morphology and 3D electrode configurations is investigated with particular emphasis on solid-state transport and resulting implications on the performance. A morphology-detailed computational modeling is presented which simulates lithium transport in disparate 3D electrode configurations. The resulting lithium concentration in the 3D electrode constructs during discharging, relaxation, and charging process reveal a local sate of charge map. This is correlated with the electrode performance. This study demonstrates the role of active particle morphology and 3D architecture on the electrode relaxation behavior, which determines the resulting concentration gradient and performance. (C) 2015 The Electrochemical Society. All rights reserved. C1 [Martin, Michael A.; Chen, Chien-Fan; Mukherjee, Partha P.; Ranjan, Devesh] Texas A&M Univ, Dept Mech Engn, College Stn, TX 77843 USA. [Pannala, Sreekanth; Turner, John A.] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. [Dietiker, Jean-Francois] Natl Energy Technol Lab, Morgantown, WV 26507 USA. [Dietiker, Jean-Francois] W Virginia Univ, Corp Res, Morgantown, WV 26507 USA. RP Martin, MA (reprint author), Texas A&M Univ, Dept Mech Engn, College Stn, TX 77843 USA. EM pmukherjee@tamu.edu; pannalas@ornl.gov; devesh.ranjan@me.gatech.edu OI Ranjan, Devesh/0000-0002-1231-9313; Turner, John/0000-0003-2521-4091 FU A&M University faculty research initiation grant; ORNL LDRD program; Oak Ridge National Laboratory FX Financial support from Texas A&M University faculty research initiation grant and ORNL LDRD program is gratefully acknowledged. PPM acknowledges Oak Ridge National Laboratory for the summer research fellowship offered to MAM during which part of the work was performed. PPM also acknowledges Malcolm Stein IV for his help with manuscript editing. NR 60 TC 3 Z9 3 U1 3 U2 25 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 EI 1945-7111 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2015 VL 162 IS 6 BP A991 EP A1002 DI 10.1149/2.0631506jes PG 12 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA CG1BZ UT WOS:000353009300029 ER PT J AU Northrop, PWC Pathak, M Rife, D De, S Santhanagopalan, S Subramanian, VR AF Northrop, Paul W. C. Pathak, Manan Rife, Derek De, Sumitava Santhanagopalan, Shriram Subramanian, Venkat R. TI Efficient Simulation and Model Reformulation of Two-Dimensional Electrochemical Thermal Behavior of Lithium-Ion Batteries SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID GENERAL ENERGY-BALANCE; HEAT-GENERATION; CAPACITY FADE; LITHIUM/POLYMER BATTERY; MATHEMATICAL-MODEL; POLYMER BATTERIES; STRESS GENERATION; MANGANESE OXIDE; INSERTION CELL; SYSTEMS AB Lithium-ion batteries are an important technology to facilitate efficient energy storage and enable a shift from petroleum based energy to more environmentally benign sources. Such systems can be utilized most efficiently if good understanding of performance can be achieved for a range of operating conditions. Mathematical models can be useful to predict battery behavior to allow for optimization of design and control, An analytical solution is ideally preferred to solve the equations of a mathematical model, as it eliminates the error that arises when using numerical techniques and is usually computationally cheap. An analytical solution provides insight into the behavior of the system and also explicitly shows the effects of different parameters on the behavior. However, most engineering models, including the majority of battery models, cannot be solved analytically due to non-linearities in the equations and state dependent transport and kinetic parameters. The numerical method used to solve the system of equations describing a battery operation can have a significant impact on the computational cost of the simulation. In this paper, a model reformulation of the porous electrode pseudo three dimensional (P3D) which significantly reduces the computational cost of lithium ion battery simulation, while maintaining high accuracy, is discussed. This reformulation enables the use of the P3D model into applications that would otherwise be too computationally expensive to justify its use, such as online control, optimization, and parameter estimation. Furthermore, the P3D model has proven to be robust enough to allow for the inclusion of additional physical phenomena as understanding improves. In this paper, the reformulated model is used to allow for more complicated physical phenomena to be considered for study, including thermal effects. (C) The Author(s) 2015. Published by ECS. All rights reserved. C1 [Northrop, Paul W. C.] CFD Res Corp, Biomed & Energy Technol, Huntsville, AL 35806 USA. [Pathak, Manan; Subramanian, Venkat R.] Univ Washington, Seattle, WA 98105 USA. [Rife, Derek; De, Sumitava] Washington Univ, Dept Energy Environm & Chem Engn, St Louis, MO 63130 USA. [Santhanagopalan, Shriram] Natl Renewable Energy Lab, Transportat & Hydrogen Syst Ctr, Golden, CO 80401 USA. [Subramanian, Venkat R.] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Northrop, PWC (reprint author), CFD Res Corp, Biomed & Energy Technol, Huntsville, AL 35806 USA. EM vsubram@uw.edu RI DE, SUMITAVA/H-6608-2016 OI DE, SUMITAVA/0000-0002-2711-082X NR 64 TC 3 Z9 3 U1 7 U2 35 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 EI 1945-7111 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2015 VL 162 IS 6 BP A940 EP A951 DI 10.1149/2.0341506jes PG 12 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA CG1BZ UT WOS:000353009300023 ER PT J AU Rinaldo, SG Gallagher, KG Long, BR Croy, JR Bettge, M Abraham, DP Bareno, J Dees, DW AF Rinaldo, Steven G. Gallagher, Kevin G. Long, Brandon R. Croy, Jason R. Bettge, Martin Abraham, Daniel P. Bareno, Javier Dees, Dennis W. TI Physical Theory of Voltage Fade in Lithium- and Manganese-Rich Transition Metal Oxides SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID MONTE-CARLO SIMULATION; LATTICE-GAS MODEL; ELECTROCHEMICAL-CELLS; ENERGY-DENSITY; 1ST PRINCIPLES; ION BATTERIES; CATHODE; INTERCALATION; ELECTRODES; HYSTERESIS AB Lithium- and manganese-rich (LMR) transition metal oxide cathodes are of interest for lithium-ion battery applications due to their increased energy density and decreased cost. However, the advantages in energy density and cost are offset, in part, due to the phenomena of voltage fade. Specifically, the voltage profiles (voltage as a function of capacity) of LMR cathodes transform from a high energy configuration to a lower energy configuration as they are repeatedly charged (Li removed) and discharged (Li inserted). We propose a physical model of voltage fade that accounts for the emergence of a low voltage Li phase due to the introduction of transition metal ion defects within a parent Li phase. The phenomenological model was re-cast in a general form and experimental LMR charge profiles were de-convoluted to extract the evolutionary behavior of various components of LMR capacitance profiles. Evolution of the voltage fade component was found to follow a universal growth curve with a maximal voltage fade capacity of approximate to 120% of the initial total capacity. (C) The Author(s) 2015. Published by ECS. All rights reserved. C1 [Rinaldo, Steven G.; Gallagher, Kevin G.; Long, Brandon R.; Croy, Jason R.; Bettge, Martin; Abraham, Daniel P.; Bareno, Javier; Dees, Dennis W.] Argonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USA. RP Rinaldo, SG (reprint author), Argonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USA. EM rinaldo@anl.gov FU Vehicle Technologies Program, Hybrid and Electric Systems; Argonne, a U.S. Department of Energy Office of Science Laboratory [DE-AC02-06CH11357] FX Support from the Vehicle Technologies Program, Hybrid and Electric Systems, in particular David Howell, Peter Faguy, and Tien Duong at the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, is gratefully acknowledged. The submitted manuscript has been created by UChicago Argonne, LLC, Operator of Argonne National Laboratory ("Argonne"). Argonne, a U.S. Department of Energy Office of Science Laboratory, is operated under Contract No. DE-AC02-06CH11357. The U.S. Government retains for itself, and others acting on its behalf, a paid-up nonexclusive, irrevocable worldwide license in said article to reproduce, prepare derivative works, distribute copies to the public, and perform publicly and display publicly, by or on behalf of the Government. We would also like to thank Mahalingam Balasubramanian for insightful discussions. NR 34 TC 6 Z9 6 U1 2 U2 33 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 EI 1945-7111 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2015 VL 162 IS 6 BP A897 EP A904 DI 10.1149/2.0181506jes PG 8 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA CG1BZ UT WOS:000353009300017 ER PT J AU Urisanga, PC Rife, D De, S Subramanian, VR AF Urisanga, Pierre Celestin Rife, Derek De, Sumitava Subramanian, Venkat R. TI Efficient Conservative Reformulation Schemes for Lithium Intercalation SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID SOLID-PHASE DIFFUSION; APPROXIMATE SOLUTION METHODS; MODEL DEVELOPMENT; POROUS-ELECTRODE; STATE DIFFUSION; INSERTION CELL; BATTERIES; DISCHARGE; DYNAMICS; EQUATION AB Porous electrode theory coupled with transport and reaction mechanisms is a widely used technique to model Li-ion batteries employing an appropriate discretization or approximation for solid phase diffusion with electrode particles. One of the major difficulties in simulating Li-ion battery models is the need to account for solid phase diffusion in a second radial dimension r, which increases the computation time/cost to a great extent. Various methods that reduce the computational cost have been introduced to treat this phenomenon, but most of them do not guarantee mass conservation. The aim of this paper is to introduce an inherently mass conserving yet computationally efficient method for solid phase diffusion based on Lobatto III A quadrature. This paper also presents coupling of the new solid phase reformulation scheme with a macro-homogeneous porous electrode theory based pseudo 20 model for Li-ion battery. (C) The Author(s) 2015. Published by ECS. All rights reserved. C1 [Urisanga, Pierre Celestin] Washington Univ, Dept Elect & Syst Engn, St Louis, MO 63130 USA. [Rife, Derek; De, Sumitava] Washington Univ, Dept Energy Environm & Chem Engn, St Louis, MO 63130 USA. [Subramanian, Venkat R.] Univ Washington, Dept Chem Engn, Seattle, WA 98195 USA. [Subramanian, Venkat R.] Pacific NW Natl Lab, Energy Proc & Mat Dept, Richland, WA 99354 USA. RP Urisanga, PC (reprint author), Washington Univ, Dept Elect & Syst Engn, St Louis, MO 63130 USA. EM vsubram@uw.edu RI DE, SUMITAVA/H-6608-2016 OI DE, SUMITAVA/0000-0002-2711-082X FU Washington University; United States Government, Advanced Research Projects Agency - Energy (ARPA-E), U.S. Department of Energy [DE-AR0000275]; McDonnell Academy Global Energy and Environment Partnership (MAGEEP) at Washington University in St. Louis FX The authors are thankful for the financial support by Washington University's Chancellor's Graduate Fellowship Program and Danforth Scholars Program, by the United States Government, Advanced Research Projects Agency - Energy (ARPA-E), U.S. Department of Energy, under award number DE-AR0000275, and by McDonnell Academy Global Energy and Environment Partnership (MAGEEP) at Washington University in St. Louis. NR 27 TC 0 Z9 0 U1 1 U2 3 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 EI 1945-7111 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2015 VL 162 IS 6 BP A852 EP A857 DI 10.1149/2.0061506jes PG 6 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA CG1BZ UT WOS:000353009300011 ER PT J AU Siegal, MP Mowry, CD Pfeifer, KB Sava Gallis, DF AF Siegal, Michael P. Mowry, Curtis D. Pfeifer, Kent B. Sava Gallis, Dorina F. TI Detecting Trihalomethanes Using Nanoporous-Carbon Coated Surface-Acoustic-Wave Sensors SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID PURGE-AND-TRAP; SAMPLING-GAS CHROMATOGRAPHY; DRINKING-WATER; CHEMICAL MICROSENSORS; ADSORPTION; DEVICES; FILMS; HYDROCARBONS; EXTRACTION AB We study nanoporous-carbon (NPC) grown via pulsed laser deposition (PLD) as a sorbent coating on 96.5-MHz surface-acoustic-wave (SAW) devices to detect trihalomethanes (THMs), regulated by products from the chemical treatment of drinking water. Using both insertion-loss and isothermal-response measurements from known quantities of chloroform, the highest vapor pressure THM, we optimize the NPC mass-density at 1.05 +/- 0.08 g/cm(3) by controlling the background argon pressure during PLD. Precise THM quantities in a chlorobenzene solvent are directly injected into a separation column and detected as the phase-angle shift of the SAW device output compared to the drive signal. Using optimized NPC-coated SAWs, we study the chloroform response as a function of operating temperatures ranging from 10-50 degrees C. Finally, we demonstrate individual responses from complex mixtures of all four THMs, with masses ranging from 10-2000 ng, after gas chromatography separation. Estimates for each THM detection limit using a simple peak-height response evaluation are 4.4 ng for chloroform and 1 ng for bromoform; using an integrated-peak area response analysis improves the detection limits to 0.73 ng for chloroform and 0.003 ng bromoform. (C) The Author(s) 2015. Published by ECS. This is an open access article distributed under the terms of the Creative Commons Attribution Non-Commercial No Derivatives 4.0 License (CC BY-NC-ND, http://creativecommons.org/licenses/by-nc-nd/4.00, which permits non-commercial reuse, distribution, and reproduction in any medium, provided the original work is not changed in any way and is properly cited. For permission for commercial reuse, please email: oa@electrochem.org. All rights reserved. C1 [Siegal, Michael P.; Mowry, Curtis D.; Pfeifer, Kent B.; Sava Gallis, Dorina F.] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Siegal, MP (reprint author), Sandia Natl Labs, POB 5800, Albuquerque, NM 87185 USA. EM mpsiega@sandia.gov RI Sava Gallis, Dorina/D-2827-2015 FU Laboratory Directed Research and Development program at Sandia National Laboratories; U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX The authors thank Don Overmyer for growing the NPC films on SAW devices, Jonathan Rivera for growing the NPC films for the mass density measurements, Lyle Brunke for growing the films for BET characterization, Art Rumpf for insertion-loss characterization, Stephen Howell for data acquisition and Labview software, and Richard Kottenstette and Alex Robinson for analyte measurements. This work is supported in part by the Laboratory Directed Research and Development program at Sandia National Laboratories. Sandia National Laboratories is a multiprogram laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Company, for the U.S. Department of Energy's National Nuclear Security Administration under Contract DE-AC04-94AL85000. NR 44 TC 1 Z9 1 U1 3 U2 10 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 EI 1945-7111 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2015 VL 162 IS 6 BP B114 EP B120 DI 10.1149/2.0381506jes PG 7 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA CG1BZ UT WOS:000353009300046 ER PT J AU Palanivelu, KM Prabhakaran, V Romani, VK Ramanujam, K AF Palanivelu, K. M. Prabhakaran, Venkateshkumar Romani, Vijay K. Ramanujam, Kothandaraman TI Controlling the Nitrogen Content of Metal-Nitrogen-Carbon Based Non-Precious-Metal Electrocatalysts via Selenium Addition SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID OXYGEN REDUCTION REACTION; PEM FUEL-CELLS; HETEROATOM-DOPED CARBON; FE-BASED CATALYSTS; FE/N/C CATALYSTS; ACTIVE-SITES; IRON; ORR; MEDIA; SPECTROSCOPY AB Non-precious metal electrocatalysts based on pyrolysed metal-nitrogen-carbon (MNC) are viewed as an inexpensive replacement for platinum-based electrocatalysts for the oxygen reduction reaction (ORR) in fuel cells. One of the drawbacks of all the reported procedures to synthesize MNC electrocatalysts is the inability to control the nitrogen content. Since the type of nitrogen present (pyridinic, pyrrolic, quaternary/graphitic) and their proportions both play a seminal role in deciding the ORR activity of the electrocatalyst. it is important to carefully study the effect of nitrogen content on electrocatalyst properties. In this study, selenium was used as a ligand to replace the nitrogen coordinated to the iron atom in the electrocatalyst, thereby imparting control on the nitrogen content. Upon introducing 14 at% of selenium, the N content of the catalyst dropped 10 3.7 wt% and the ORR activity reached a maximum of 7.2 mA cm(-2) at 0.8 V vs. RHE. We demonstrated the need for iron to complete the active site: upon complexing the iron site with bipyridine, ethylene diammine and oxalic acid in IN H2SO4, the overpotential toward the ORR increased by similar to 60 mV, similar to 140 mV and similar to 140 mV respectively at 2 mA cm(-2). (C) 2015 The Electrochemical Society. All rights reserved. C1 [Palanivelu, K. M.; Ramanujam, Kothandaraman] Indian Inst Technol, Dept Chem, Madras 600036, Tamil Nadu, India. [Prabhakaran, Venkateshkumar; Romani, Vijay K.] IIT, Dept Chem & Biol Engn, Chicago, IL 60616 USA. [Prabhakaran, Venkateshkumar] Pacific NW Natl Lab, Richland, WA 99354 USA. RP Palanivelu, KM (reprint author), Indian Inst Technol, Dept Chem, Madras 600036, Tamil Nadu, India. EM rkraman@iitm.ac.in RI Prabhakaran, Venkateshkumar/C-5023-2009; Ramani, Vijay/A-5164-2010 OI Prabhakaran, Venkateshkumar/0000-0001-6692-6488; Ramani, Vijay/0000-0002-6132-8144 FU ISRO-IITM space cell [CHY/11-12/351/ISRO/KOTH] FX We thank ISRO-IITM space cell for funding this project (CHY/11-12/351/ISRO/KOTH), thank Prof. V Munichandraiah from IISc Bangalore for TEM work, IIT Madras for infrastructure and facilities and Prof. Vijay Ramani and his student from IIT Chicago, USA for XPS studies. We thank Prof. Scott C. Barton from Michigan State University for supplying Ketjenblack 600JD carbon in kind. NR 43 TC 9 Z9 9 U1 3 U2 32 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 EI 1945-7111 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2015 VL 162 IS 6 BP F475 EP F482 DI 10.1149/2.0101506jes PG 8 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA CG1BZ UT WOS:000353009300071 ER PT J AU Yim, SD Chung, HT Chlistunoff, J Kim, DS Fujimoto, C Yang, TH Kim, YS AF Yim, Sung-Dae Chung, Hoon T. Chlistunoff, Jerzy Kim, Dae-Sik Fujimoto, Cy Yang, Tae-Hyun Kim, Yu Seung TI A Microelectrode Study of Interfacial Reactions at the Platinum-Alkaline Polymer Interface SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID MEMBRANE FUEL-CELLS; OXYGEN REDUCTION KINETICS; ANION-EXCHANGE MEMBRANES; DIELECTRIC-PROPERTIES; HYDRATION STRUCTURE; NAFION INTERFACE; ELECTROLYTE; IONOMER; PERFORMANCE; STABILITY AB Hydrogen oxidation (HOR) and oxygen reduction (ORR) reactions at the platinum/alkaline ionomer interface were investigated using two different alkaline polymer electrolytes, i.e., benzyl-trimethyl ammonium tethered poly(phenylene) (ATM-PP) and phenyl-pentamethyl guanidinium tethered perfluorinated polymer (M-Nafion-FA-TMG). Substantial inhibition of HOR was taking place at the platinum-ATM-PP interface due to the possible cationic group adsorption of ATM-PP, whereas the reaction was virtually unaffected at the platinum-M-Nafion-FA-TMG interface after high anodic potential preconditioning. Moreover, the apparent ORR activity of platinum coated with M-Nafion-FA-TMG was found higher than that in 0.1 M tetra methyl guanidinium solution. In addition, the oxygen permeability of M-Nafion-FA-TMG was found to be similar to 2.5 times higher than that of ATM-PP. The above properties of the perfluorinated polymer make it a very promising ionomeric binder for the use in both anode and cathode of alkaline membrane fuel cells. (C) The Author(s) 2015. Published by ECS. This is an open access article distributed under the terms of the Creative Commons Attribution 4.0 License (CC BY, http://creativecommons.org/licenses/by/4.0/), which permits unrestricted reuse of the work in any medium, provided the original work is properly cited. All rights reserved. C1 [Yim, Sung-Dae; Chung, Hoon T.; Chlistunoff, Jerzy; Kim, Dae-Sik; Kim, Yu Seung] Los Alamos Natl Lab, Mat Synth & Integrated Devices Grp, Los Alamos, NM 87545 USA. [Yim, Sung-Dae; Yang, Tae-Hyun] Korea Inst Energy Res, Fuel Cell Lab, Taejon 305343, South Korea. [Fujimoto, Cy] Sandia Natl Labs, Organ Mat Sci, Albuquerque, NM 87185 USA. RP Yim, SD (reprint author), Los Alamos Natl Lab, Mat Synth & Integrated Devices Grp, POB 1663, Los Alamos, NM 87545 USA. EM yskim@lanl.gov OI Chung, Hoon/0000-0002-5367-9294 FU US Department of Energy by Los Alamos National Security LLC [DE-AC52-06NA25396]; US DOE Fuel Cell Technologies Program; Korea Institute of Energy Research, South Korea [B5-2415-01]; Korea Institute of Energy Technology Evaluation and Planning (KETEP); Ministry of Trade, Industry & Energy, South Korea [20138520030780] FX Los Alamos National Laboratory is operated for the US Department of Energy by Los Alamos National Security LLC under Contract DE-AC52-06NA25396. We thank US DOE Fuel Cell Technologies Program, Technology Development Manager Dr. Nancy Garland, for financial support. S.D.Y. acknowledges financial support from Korea Institute of Energy Research, South Korea (B5-2415-01), and from the International Collaborative Energy Technology R&D Program of the Korea Institute of Energy Technology Evaluation and Planning (KETEP) granted financial resource from the Ministry of Trade, Industry & Energy, South Korea (20138520030780). NR 44 TC 4 Z9 4 U1 8 U2 38 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 EI 1945-7111 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2015 VL 162 IS 6 BP F499 EP F506 DI 10.1149/2.0151506jes PG 8 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA CG1BZ UT WOS:000353009300074 ER PT S AU Fereidouni, F Datta-Mitra, A Demos, S Levenson, R AF Fereidouni, Farzad Datta-Mitra, Ananya Demos, Stavros Levenson, Richard BE Alfano, RR Demos, SG TI Microscopy with UV Surface Excitation (MUSE) for slide-free histology and pathology imaging SO OPTICAL BIOPSY XIII: TOWARD REAL-TIME SPECTROSCOPIC IMAGING AND DIAGNOSIS SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Optical Biopsy XIII: Toward Real-Time Spectroscopic Imaging and Diagnosis CY FEB 10-11, 2015 CL San Francisco, CA SP SPIE, Bayspec Inc, Coherent Inc, Corning Inc, Energy Res Co, Fianium Ltd, Hamamatsu Corp, Intuit Surg Corp, LEUKOS, NKT Photon A S, PerkinElmer Inc, ThorLabs Inc DE Fluorescence imaging; microscopy; histology AB A novel microscopy method that takes advantage of shallow photon penetration using ultraviolet-range excitation and exogenous fluorescent stains is described. This approach exploits the intrinsic optical sectioning function when exciting tissue fluorescence from superficial layers to generate images similar to those obtainable from a physically thin-sectioned tissue specimen. UV light in the spectral range from roughly 240-275 nm penetrates only a few microns into the surface of biological specimens, thus eliminating out-of-focus signals that would otherwise arise from deeper tissue layers. Furthermore, UV excitation can be used to simultaneously excite fluorophores emitting across a wide spectral range. The sectioning property of the UV light (as opposed to more conventional illumination in the visible range) removes the need for physical or more elaborate optical sectioning approaches, such as confocal, nonlinear or coherent tomographic methods, to generate acceptable axial resolution. Using a tunable laser, we investigated the effect of excitation wavelength in the 230-350 nm spectral range on excitation depth. The results reveal an optimal wavelength range and suggest that this method can be a fast and reliable approach for rapid imaging of tissue specimens. Some of this range is addressable by currently available and relatively inexpensive LED light sources. MUSE may prove to be a good alternative to conventional, time-consuming, histopathology procedures. C1 [Fereidouni, Farzad; Datta-Mitra, Ananya; Levenson, Richard] Univ Calif Davis, Pathol & Lab Med, Sacramento, CA 95817 USA. [Demos, Stavros] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. RP Fereidouni, F (reprint author), Univ Calif Davis, Pathol & Lab Med, Sacramento, CA 95817 USA. EM levenson@ucdavis.edu NR 8 TC 1 Z9 1 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 978-1-62841-408-0 J9 PROC SPIE PY 2015 VL 9318 AR 93180F DI 10.1117/12.2080408 PG 6 WC Engineering, Biomedical; Optics; Radiology, Nuclear Medicine & Medical Imaging; Spectroscopy SC Engineering; Optics; Radiology, Nuclear Medicine & Medical Imaging; Spectroscopy GA BC5QC UT WOS:000353479900011 ER PT J AU Kirshenbaum, KC Bock, DC Brady, AB Marschilok, AC Takeuchi, KJ Takeuchi, ES AF Kirshenbaum, Kevin C. Bock, David C. Brady, Alexander B. Marschilok, Amy C. Takeuchi, Kenneth J. Takeuchi, Esther S. TI Electrochemical reduction of an Ag2VO2PO4 particle: dramatic increase of local electronic conductivity SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID VANADIUM PHOSPHORUS OXIDE; X-RAY-DIFFRACTION; MECHANISTIC INSIGHTS; BATTERY APPLICATIONS; CATHODE MATERIAL; DISCHARGE; PERFORMANCE; DISSOLUTION; KINETICS; DEVICES AB Previously, we reported that electrodes containing silver vanadium phosphate (Ag2VO2PO4) powder exhibit a 15000 fold increase in conductivity after discharge, concurrent with the formation of silver metal. In this study, in order to disentangle the complex nature of electrodes composed of electroactive powders, an electrochemical reduction of individual particles of Ag2VO2PO4 was conducted, to more directly probe the intrinsic materials properties of Ag2VO2PO4. Specifically, individual particle conductivity data from a nanoprobe system combined with SEM and optical imaging results revealed that the depth of discharge within an Ag2VO2PO4 particle is closely linked to the conductivity increase. Notably, the formation of silver metal may affect both inter-and intraparticle conductivity of the Ag2VO2PO4 material. C1 [Kirshenbaum, Kevin C.; Takeuchi, Esther S.] Brookhaven Natl Lab, Upton, NY 11973 USA. [Bock, David C.; Marschilok, Amy C.; Takeuchi, Kenneth J.; Takeuchi, Esther S.] SUNY Stony Brook, Dept Chem, Stony Brook, NY 11794 USA. [Brady, Alexander B.; Marschilok, Amy C.; Takeuchi, Kenneth J.; Takeuchi, Esther S.] SUNY Stony Brook, Dept Mat Sci & Engn, Stony Brook, NY 11794 USA. RP Marschilok, AC (reprint author), SUNY Stony Brook, Dept Chem, Stony Brook, NY 11794 USA. EM amy.marschilok@stonybrook.edu; kenneth.takeuchi.1@stonybrook.edu; esther.takeuchi@stonybrook.edu FU Center for Mesoscale Transport Properties; Energy Frontier Research Center; U.S. Department of Energy, Office of Science, Basic Energy Sciences [DE-SC0012673]; U.S. Department of Energy, Office of Basic Energy Science [DE-AC02-98CH10886]; Brookhaven National Laboratory; Gertrude and Maurice Goldhaber Distinguished Fellowship Program FX This work was supported as part of the Center for Mesoscale Transport Properties, an Energy Frontier Research Center supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, under award #DE-SC0012673. The use of the Center for Functional Nanomaterials was supported by the U.S. Department of Energy, Office of Basic Energy Science under contract number DE-AC02-98CH10886. K. Kirshenbaum acknowledges Postdoctoral support from Brookhaven National Laboratory and the Gertrude and Maurice Goldhaber Distinguished Fellowship Program. The authors thank Qing Zhang for assistance with scanning electron microscopy. NR 33 TC 4 Z9 4 U1 3 U2 30 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2015 VL 17 IS 17 BP 11204 EP 11210 DI 10.1039/c5cp00961h PG 7 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA CG5NN UT WOS:000353338800011 PM 25827353 ER PT J AU DeCaluwe, SC Dhar, BM Huang, L He, Y Yang, K Owejan, JP Zhao, Y Talin, AA Dura, JA Wang, H AF DeCaluwe, S. C. Dhar, B. M. Huang, L. He, Y. Yang, K. Owejan, J. P. Zhao, Y. Talin, A. A. Dura, J. A. Wang, H. TI Pore collapse and regrowth in silicon electrodes for rechargeable batteries SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID LITHIUM-ION BATTERIES; SOLID-STATE AMORPHIZATION; ATOMIC LAYER DEPOSITION; IN-SITU OBSERVATION; AMORPHOUS-SILICON; NEUTRON REFLECTOMETRY; HIGH-CAPACITY; ELECTROCHEMICAL PERFORMANCE; STRUCTURAL-CHANGES; VOLUME EXPANSION AB Structure and composition of an 11 nm thick amorphous silicon (a-Si) thin film anode, capped with 4 nm of alumina are measured, in operando, by neutron reflectivity (NR) and electrochemical impedance spectroscopy in a lithium half-cell. NR data are analyzed to quantify the a-Si thickness and composition at various states of charge over six cycles. The a-Si anode expands and contracts upon lithiation and delithiation, respectively, while maintaining its integrity and low interfacial roughness (<= 1.6 nm) throughout the cycling. The apparently non-linear expansion of the a-Si layer volume versus lithium content agrees with previous thin-film a-Si anode studies. However, a proposed pore collapse and regrowth (PCRG) mechanism establishes that the solid domains in the porous LixSi film expand linearly with Li content at 8.48 cm(3) mol(-1) Li, similar to crystalline Si. In the PCRG model, porosity is first consumed by expansion of solid domains upon lithiation, after which the film as a whole expands. Porosity is reestablished at 5-28% upon delithiation. Data show that the alumina protective layer on the a-Si film functions as an effective artificial solid electrolyte interphase (SEI), maintaining its structural integrity, low interfacial roughness, and relatively small transport resistance. No additional spontaneously-formed SEI is observed in this study. C1 [DeCaluwe, S. C.] Colorado Sch Mines, Dept Mech Engn, Golden, CO 80401 USA. [DeCaluwe, S. C.; Dura, J. A.] NIST, Ctr Neutron Res, Gaithersburg, MD 20899 USA. [DeCaluwe, S. C.; Wang, H.] Univ Maryland, Dept Mat Sci & Engn, College Pk, MD 20742 USA. [Dhar, B. M.; Huang, L.; He, Y.; Yang, K.; Wang, H.] SUNY Binghamton, Inst Mat Res, Binghamton, NY USA. [Dhar, B. M.; Huang, L.; He, Y.; Yang, K.; Wang, H.] SUNY Binghamton, Dept Mech Engn, Binghamton, NY USA. [Dhar, B. M.; Wang, H.] NIST, Mat Measurement Lab, Gaithersburg, MD 20899 USA. [He, Y.; Zhao, Y.] Univ Georgia, Dept Phys & Astron, Athens, GA 30602 USA. [Owejan, J. P.] SUNY Alfred, Dept Mech & Elect Engn Technol, Alfred, NY 14802 USA. [Talin, A. A.] NIST, Ctr Nanoscale Sci & Technol, Gaithersburg, MD 20899 USA. [Talin, A. A.] Sandia Natl Labs, Livermore, CA USA. RP Dura, JA (reprint author), NIST, Ctr Neutron Res, Gaithersburg, MD 20899 USA. EM jdura@nist.gov; wangh@umd.edu RI Dura, Joseph/B-8452-2008; Zhao, Yiping/A-4968-2008 OI Dura, Joseph/0000-0001-6877-959X; FU NIST; General Motors; National Research Council; US Army Research Laboratory [W911NF-10-2-0107]; San Corporation, a Lockheed Martin Company, for the U.S. DOE National Nuclear Security Administration [DE-AC04-94AL85000]; U.S. Department of Energy, Office of Science, and Office of Basic Energy Sciences [DESC0001160] FX HW acknowledges NIST and General Motors for their generous financial support. SCD thanks the National Research Council for funding via the Research Associates Program. YPH and YPZ were supported by US Army Research Laboratory with the contract number of W911NF-10-2-0107. Sandia is a multi-program laboratory operated by San Corporation, a Lockheed Martin Company, for the U.S. DOE National Nuclear Security Administration under Contract DE-AC04-94AL85000. AAT acknowledges partial support for data analysis and writing of the manuscript by Science of Precision Multifunctional Nanostructures for Electrical Energy Storage (NEES), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, and Office of Basic Energy Sciences under DESC0001160. NR 62 TC 4 Z9 4 U1 8 U2 66 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2015 VL 17 IS 17 BP 11301 EP 11312 DI 10.1039/c4cp06017b PG 12 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA CG5NN UT WOS:000353338800023 PM 25839065 ER PT J AU Perticaroli, S Russo, D Paolantoni, M Gonzalez, MA Sassi, P Nickels, JD Ehlers, G Comez, L Pellegrini, E Fioretto, D Morresi, A AF Perticaroli, S. Russo, D. Paolantoni, M. Gonzalez, M. A. Sassi, P. Nickels, J. D. Ehlers, G. Comez, L. Pellegrini, E. Fioretto, D. Morresi, A. TI Painting biological low-frequency vibrational modes from small peptides to proteins SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID INELASTIC NEUTRON-SCATTERING; DEPOLARIZED LIGHT-SCATTERING; METHYL-GROUP DYNAMICS; WATER HYDROGEN-BOND; MOLECULAR-CRYSTALS; GLOBULAR-PROTEINS; HYDRATION WATER; BOSON PEAK; MONOSUBSTITUTED AMIDES; INTERNAL-ROTATION AB Protein low-frequency vibrational modes are an important portion of a proteins' dynamical repertoire. Yet, it is notoriously difficult to isolate specific vibrational features in the spectra of proteins. Given an appropriately chosen model peptide, and using different experimental conditions, we can simplify the system and gain useful insights into the protein vibrational properties. Combining neutron scattering, depolarized light scattering, and molecular dynamics simulations, we analyse the low frequency vibrations of biological molecules, comparing the results from a small globular protein, lysozyme, and an amphiphilic peptide, NALMA, both in solution and in powder states. Lysozyme and NALMA present similar spectral features in the frequency range between 1 and 10 THz. With the aid of MD simulations, we assign the spectral features to methyl groups' librations (1-5 THz) and hindered torsions (5-10 THz) in NALMA. Our data also show that, while proteins display boson peak vibrations in both powder and solution forms, NALMA exhibits boson peak vibrations in powder form only. This provides insight into the nature of this feature, suggesting a connection of BP collective motions to a characteristic length scale of heterogeneities present in the system. These results provide context for the use of model peptide systems to study protein dynamics; demonstrating both their utility, and the great care that has to be used in extrapolating results observed in powder to solutions. C1 [Perticaroli, S.; Nickels, J. D.] Oak Ridge Natl Lab, Joint Inst Neutron Sci, Oak Ridge, TN 37831 USA. [Perticaroli, S.] Oak Ridge Natl Lab, Div Chem & Mat Sci, Oak Ridge, TN 37831 USA. [Perticaroli, S.; Nickels, J. D.] Univ Tennessee, Dept Chem, Knoxville, TN 37996 USA. [Russo, D.] Inst Max Von Laue Paul Langevin, CNR IOM, Grenoble, France. [Russo, D.] Univ Lyon 1, Inst Lumiere Mat, F-69622 Villeurbanne, France. [Paolantoni, M.; Sassi, P.; Morresi, A.] Univ Perugia, Dipartimento Chim Biol & Biotecnol, I-06123 Perugia, Italy. [Gonzalez, M. A.; Pellegrini, E.] Inst Max Von Laue Paul Langevin, F-38042 Grenoble, France. [Ehlers, G.] Oak Ridge Natl Lab, Quantum Condensed Matter Div, Oak Ridge, TN 37831 USA. [Comez, L.] Univ Perugia, Dipartimento Fis & Geol, IOM CNR, I-06123 Perugia, Italy. [Comez, L.; Fioretto, D.] Univ Perugia, Dipartimento Fis & Geol, I-06123 Perugia, Italy. [Fioretto, D.] Univ Perugia, Ctr Eccellenza Mat Innovat Nanostrutturati, I-06123 Perugia, Italy. RP Perticaroli, S (reprint author), Oak Ridge Natl Lab, Joint Inst Neutron Sci, Oak Ridge, TN 37831 USA. EM spertica@utk.edu; russo@ill.fr RI Sassi, Paola/F-1141-2014; Morresi, Assunta/M-7359-2014; Instrument, CNCS/B-4599-2012; Paolantoni, Marco /G-1646-2014; Ehlers, Georg/B-5412-2008; Nickels, Jonathan/I-1913-2012; Gonzalez, Miguel/R-8330-2016 OI Sassi, Paola/0000-0002-4920-2784; Morresi, Assunta/0000-0002-0481-6424; Paolantoni, Marco /0000-0002-6266-3497; Ehlers, Georg/0000-0003-3513-508X; Nickels, Jonathan/0000-0001-8351-7846; Gonzalez, Miguel/0000-0002-3478-0215 FU MIUR-PRIN; Scientific User Facilities Division, Office of Basic Energy Sciences, U. S. Department of Energy FX S.P. acknowledges the Computing for Science (CS) group at Institut Laue-Langevin (Grenoble, France); M.P. acknowledges support from MIUR-PRIN 2010-2011. Research at the Spallation Neutron Source, Oak Ridge National Laboratory, was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U. S. Department of Energy. NR 63 TC 5 Z9 5 U1 5 U2 34 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2015 VL 17 IS 17 BP 11423 EP 11431 DI 10.1039/c4cp05388e PG 9 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA CG5NN UT WOS:000353338800036 PM 25853990 ER PT J AU Pham, HH Wang, LW AF Pham, Hieu H. Wang, Lin-Wang TI Electronic structures and current conductivities of B, C, N and F defects in amorphous titanium dioxide SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID PHOTOCATALYTIC ACTIVITY; DOPED TIO2; ANATASE; NANOMATERIALS; IRRADIATION; SIMULATION; OXIDATION; COATINGS; POWDERS; ORIGIN AB Although titanium dioxide (TiO2) has been extensively studied and widely used in energy and environmental areas, the amorphous form and its related defect properties are poorly understood. Recent studies, however, have emphasized the crucial role of amorphousness in producing competitively good performances in photochemical applications. In this work we have investigated for the first time the effects of various dopants (B, C, N and F) on charge carrier transport in amorphous titanium dioxide (a-TiO2), given that doping is a common technique used to tune the electronic properties of semiconductors, and that the existence of these impurities could also be unintentionally introduced during the synthesis process. The a-TiO2 model was obtained using a classical molecular dynamics method, followed by density-functional theory calculations (DFT + U, with Hubbard correction term U) on electronic structures and defect states. The formation of these impurity defects in a-TiO2 was found to be energetically more favorable by several eV than their crystal counterparts (in rutile). The contributions of these defect states to the charge transfer processes were examined by means of Marcus theory. C1 [Wang, Lin-Wang] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Joint Ctr Artificial Photosynth, Berkeley, CA 94720 USA. Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. RP Wang, LW (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Joint Ctr Artificial Photosynth, Berkeley, CA 94720 USA. EM lwwang@lbl.gov FU Office of Science of the U.S. Department of Energy [DE-SC0004993] FX This material is based on the work performed by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the U.S. Department of Energy under Award number DE-SC0004993. We used the resource of the National Energy Research Scientific Computing center (NERSC) located in the Lawrence Berkeley National Laboratory. NR 51 TC 5 Z9 5 U1 4 U2 25 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2015 VL 17 IS 17 BP 11908 EP 11913 DI 10.1039/c5cp00890e PG 6 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA CG5NN UT WOS:000353338800085 PM 25872146 ER PT J AU Fu, SF Yang, GH Zhou, YZ Pan, HB Wai, CM Du, D Lin, YH AF Fu, Shaofang Yang, Guohai Zhou, Yazhou Pan, Horng-Bin Wai, Chien M. Du, Dan Lin, Yuehe TI Ultrasonic enhanced synthesis of multi-walled carbon nanotube supported Pt-Co bimetallic nanoparticles as catalysts for the oxygen reduction reaction SO RSC ADVANCES LA English DT Article ID MEMBRANE FUEL-CELL; ALLOY CATALYSTS; ELECTROCATALYSTS; PERFORMANCE; NI; FE; HYDROGENOLYSIS; STABILITY; CHEMICALS; LIGNIN AB Carbon material supported bi-or tri-metallic nanoparticles were usually used to replace noble metals, such as platinum, for improving catalytic performance and reducing the cost. In this paper, a carboxylate-functionalized multi-walled carbon nanotube supported bimetallic platinum-cobalt nanoparticles catalyst was synthesized using a simple one-step ultrasonic method. Electrochemical experiments showed that this catalyst exhibited excellent electrocatalytic activity in acid solution for the oxygen reduction reaction. In detail, the onset potential and half-wave potential of this catalyst positively shifted compared with the commercial platinum/carbon catalyst. The as-prepared catalyst also presented a high mass activity. Additionally, it showed a four-electron reduction pathway for the oxygen reduction reaction and exhibited better stability (about 82.8% current density was maintained) than platinum/carbon during the current durability test. C1 [Fu, Shaofang; Yang, Guohai; Zhou, Yazhou; Du, Dan; Lin, Yuehe] Washington State Univ, Dept Mech & Mat Engn, Pullman, WA 99163 USA. [Pan, Horng-Bin; Wai, Chien M.] Univ Idaho, Dept Chem, Moscow, ID 83844 USA. [Lin, Yuehe] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Lin, YH (reprint author), Washington State Univ, Dept Mech & Mat Engn, Pullman, WA 99163 USA. EM yuehe.lin@wsu.edu RI Lin, Yuehe/D-9762-2011; FU, SHAOFANG/D-2328-2016 OI Lin, Yuehe/0000-0003-3791-7587; FU, SHAOFANG/0000-0002-7871-6573 FU Washington State University, USA; DOE by Battelle [DE-AC05-76RL01830] FX This work was supported by a startup fund of Washington State University, USA. We thank Franceschi Microscopy & Image Center at Washington State University for TEM measurements. Pacific Northwest National Laboratory is a multi-program national laboratory operated for DOE by Battelle under Contract DE-AC05-76RL01830. NR 37 TC 8 Z9 8 U1 2 U2 29 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2046-2069 J9 RSC ADV JI RSC Adv. PY 2015 VL 5 IS 41 BP 32685 EP 32689 DI 10.1039/c5ra02549d PG 5 WC Chemistry, Multidisciplinary SC Chemistry GA CG3GH UT WOS:000353166300074 ER PT J AU Xi, JX Kim, J Si, XHA Corley, RA Kabilan, S Wang, SY AF Xi, Jinxiang Kim, JongWon Si, Xiuhua A. Corley, Richard A. Kabilan, Senthil Wang, Shengyu TI CFD Modeling and Image Analysis of Exhaled Aerosols due to a Growing Bronchial Tumor: towards Non-Invasive Diagnosis and Treatment of Respiratory Obstructive Diseases SO THERANOSTICS LA English DT Article DE Aerosol breath test; computer aided diagnosis; theranostics; aerosol fingerprint; fractal dimension; obstructive respiratory diseases ID UPPER TRACHEOBRONCHIAL AIRWAYS; BREATH CONDENSATE; PARTICLE DEPOSITION; OXIDATIVE STRESS; BOLUS DISPERSION; FRACTAL GEOMETRY; LUNG PATHOLOGY; CANCER; NANOPARTICLE; MORPHOMETRY AB Diagnosis and prognosis of tumorigenesis are generally performed with CT, PET, or biopsy. Such methods are accurate, but have the limitations of high cost and posing additional health risks to patients. In this study, we introduce an alternative computer aided diagnostic tool that can locate malignant sites caused by tumorigenesis in a non-invasive and low-cost way. Our hypothesis is that exhaled aerosol distribution is unique to lung structure and is sensitive to airway structure variations. With appropriate approaches, it is possible to locate the disease site, determine the disease severity, and subsequently formulate a targeted drug delivery plan to treat the disease. This study numerically evaluated the feasibility of the proposed breath test in an image-based lung model with varying pathological stages of a bronchial squamous tumor. Large eddy simulations and a Lagrangian tracking approach were used to model respiratory airflows and aerosol dynamics. Respirations of tracer aerosols of 1 mu m at a flow rate of 20 L/min were simulated, with the distributions of exhaled aerosols recorded on a filter at the mouth exit. Aerosol patterns were quantified with multiple analytical techniques such as concentration disparity, spatial scanning and fractal analysis. We demonstrated that a growing bronchial tumor induced notable variations in both the airflow and exhaled aerosol distribution. These variations became more apparent with increasing tumor severity. The exhaled aerosols exhibited distinctive pattern parameters such as spatial probability, fractal dimension, and multifractal spectrum. Results of this study show that morphometric measures of the exhaled aerosol pattern can be used to detect and monitor the pathological states of respiratory diseases in the upper airway. The proposed breath test also has the potential to locate the site of the disease, which is critical in developing a personalized, site-specific drug delivery protocol. C1 [Xi, Jinxiang; Kim, JongWon] Cent Michigan Univ, Sch Engn & Technol, Mt Pleasant, MI 48858 USA. [Si, Xiuhua A.] Calif Baptist Univ, Dept Mech Engn, Riverside, CA 92504 USA. [Corley, Richard A.; Kabilan, Senthil] Pacific NW Natl Lab, Syst Toxicol & Exposure Sci, Richland, WA 99352 USA. [Wang, Shengyu] Xian Med Univ, Affiliated Hosp 1, Dept Pulm & Crit Care Med, Xian 710077, Shaanxi, Peoples R China. [Wang, Shengyu] Mayo Clin, Dept Anesthesiol, Rochester, MN 55905 USA. RP Xi, JX (reprint author), Cent Michigan Univ, Sch Engn & Technol, 1200 South Franklin St, Mt Pleasant, MI 48858 USA. EM xi1j@cmich.edu NR 51 TC 3 Z9 3 U1 3 U2 12 PU IVYSPRING INT PUBL PI LAKE HAVEN PA PO BOX 4546, LAKE HAVEN, NSW 2263, AUSTRALIA SN 1838-7640 J9 THERANOSTICS JI Theranostics PY 2015 VL 5 IS 5 BP 443 EP 455 DI 10.7150/thno.11107 PG 13 WC Medicine, Research & Experimental SC Research & Experimental Medicine GA CG1VQ UT WOS:000353063800001 PM 25767612 ER PT J AU Drewry, JL Choi, CY An, L Gharagozloo, PE AF Drewry, J. L. Choi, C. Y. An, L. Gharagozloo, P. E. TI A COMPUTATIONAL FLUID DYNAMICS MODEL OF ALGAL GROWTH: DEVELOPMENT AND VALIDATION SO TRANSACTIONS OF THE ASABE LA English DT Article DE Algae; Biofuels; Computational fluid dynamics (CFD) ID RACEWAY; PHOTOSYNTHESIS; MICROALGAE; RADIATION; PH AB Biofuels derived from algae are becoming an increasingly viable alternative to petroleum-based fuels; however, research and development in the field must continue to advance the technology before biofuels can be produced in an economical and environmentally friendly manner. Unlike with photobioreactors, there is no generally accepted model for evaluating the growth of algae in open raceways because algal growth involves a large number of variables. For this reason, computational fluid dynamics (CFD) could prove to be a valuable and effective tool for the design, optimization, and operation of large-scale raceway ponds under local environmental conditions. CFD can elucidate and quantify the complex sets of variables that govern heat, mass, and flow patterns within the pond and provide spatiotemporal data concerning algal concentration and other water quality variables, such as light and temperature. The corresponding outcomes will enable designers to create more efficient ponds and more accurately predict growth under a variety of scenarios, as well as optimize the pond's operation in order to produce the maximum amount of biomass possible within a given locality. The present study focuses on developing user-defined functions capable of capturing key parameters, verifying the CFD outcomes against existing experimental data, providing computational solutions, and assessing the sensitivity of the model. C1 [Drewry, J. L.; Choi, C. Y.] Univ Wisconsin, Dept Biol Syst Engn, Madison, WI 53706 USA. [An, L.] Univ Arizona, Dept Agr & Biosyst Engn, Tucson, AZ USA. [Gharagozloo, P. E.] Sandia Natl Labs, Thermal Fluid Sci & Engn, Livermore, CA USA. RP Choi, CY (reprint author), Univ Wisconsin, 460 Henry Mall, Madison, WI 53706 USA. EM cchoi22@wisc.edu FU U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX Sandia National Laboratories is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy's National Nuclear Security Administration under Contract No. DE-AC04-94AL85000. NR 23 TC 2 Z9 2 U1 3 U2 15 PU AMER SOC AGRICULTURAL & BIOLOGICAL ENGINEERS PI ST JOSEPH PA 2950 NILES RD, ST JOSEPH, MI 49085-9659 USA SN 2151-0032 EI 2151-0040 J9 T ASABE JI Trans. ASABE PY 2015 VL 58 IS 2 BP 203 EP 213 PG 11 WC Agricultural Engineering SC Agriculture GA CG3AX UT WOS:000353149900003 ER PT J AU Mistry, KK Pol, VG Thackeray, MM Wen, JG Miller, DJ Erdemir, A AF Mistry, Kuldeep K. Pol, Vilas G. Thackeray, Michael M. Wen, Jianguo Miller, Dean J. Erdemir, Ali TI Synthesis and Tribology of Micro-Carbon Sphere Additives for Enhanced Lubrication SO TRIBOLOGY TRANSACTIONS LA English DT Article DE Carbon; Spheres; Additive; Lubricant; Tribology; Tribofilm ID SLIDING STEEL SURFACES; FRICTION; GRAPHITE; GRAPHENE; WEAR; CARBONIZATION; POLYETHYLENE; PRESSURE; ONIONS AB Poor or inefficient lubrication often gives rise to high friction and wear losses in machine components, which adversely affect their performance, efficiency, and durability. Many approaches are being explored to enhance the antifriction and antiwear properties of sliding machine components. In this study, the antifriction and antiwear properties of carbon spheres, synthesized from plastic waste by an autogenic process, were investigated as an additive to a poly-alpha-olefin (PAO-4 grade) oil. When dispersed at 1 wt% concentration, the carbon spheres reduced both friction and wear under boundary-lubricated sliding conditions. In particular, the reduction in wear was quite dramatic and appeared to be enabled by the formation of a fairly thick (approximate to 200 nm) carbon-rich boundary film, the formation of which is attributed to tribochemical interactions between the carbon particles and sliding contact surfaces. C1 [Mistry, Kuldeep K.; Pol, Vilas G.; Thackeray, Michael M.; Wen, Jianguo; Miller, Dean J.; Erdemir, Ali] Argonne Natl Lab, Lemont, IL 60439 USA. RP Mistry, KK (reprint author), Argonne Natl Lab, Lemont, IL 60439 USA. FU U.S. Department of Energy (DOE); Argonne, a U.S. Department of Energy Office of Science laboratory [DE-AC02-06CH11357] FX This research was supported by the U.S. Department of Energy (DOE). Use of DOE's facilities at the Center for Nanoscale Materials and Electron Microscopy Center at Argonne National Laboratory, both of which are supported by the Office of Science, and the XPS, AES, FIB, and TEM facilities at the Frederick Seitz Materials Research Laboratory, University of Illinois at Urbana-Champaign, is gratefully acknowledged. The submitted manuscript has been created by UChicago Argonne, LLC, Operator of Argonne National Laboratory ("Argonne"). Argonne, a U.S. Department of Energy Office of Science laboratory, is operated under Contract No. DE-AC02-06CH11357. The U.S. Government retains for itself, and others acting on its behalf, a paid-up nonexclusive, irrevocable worldwide license in said article to reproduce, prepare derivative works, distribute copies to the public, and perform publicly and display publicly, by or on behalf of the Government. NR 29 TC 5 Z9 5 U1 3 U2 31 PU TAYLOR & FRANCIS INC PI PHILADELPHIA PA 530 WALNUT STREET, STE 850, PHILADELPHIA, PA 19106 USA SN 1040-2004 EI 1547-397X J9 TRIBOL T JI Tribol. Trans. PY 2015 VL 58 IS 3 BP 474 EP 480 DI 10.1080/10402004.2014.983252 PG 7 WC Engineering, Mechanical SC Engineering GA CG8TT UT WOS:000353586400009 ER PT S AU Yang, Z Albrecht, AR Cederberg, JG Sheik-Bahae, M AF Yang, Zhou Albrecht, Alexander R. Cederberg, Jeffrey G. Sheik-Bahae, Mansoor BE Guina, M TI DBR-free optically pumped semiconductor disk lasers SO VERTICAL EXTERNAL CAVITY SURFACE EMITTING LASERS (VECSELS) V SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Vertical External Cavity Surface Emitting Lasers (VECSELs) V CY FEB 09-10, 2015 CL San Francisco, CA SP SPIE, Coherent Inc DE Semiconductor Disk Laser; Optically Pumped Semiconductor Laser; VECSEL; DBR-free ID SURFACE-EMITTING LASERS; INTRACAVITY; VECSEL AB Optically pumped semiconductor disk lasers (SDLs) provide high beam quality with high average-power power at designer wavelengths. However, material choices are limited by the need for a distributed Bragg reflector (DBR), usually monolithically integrated with the active region. We demonstrate DBR-free SDL active regions, which have been lifted off and bonded to various transparent substrates. For an InGaAs multi-quantum well sample bonded to a diamond window heat spreader, we achieved CW lasing with an output power of 2 W at 1150 nm with good beam quality. C1 [Yang, Zhou; Albrecht, Alexander R.; Sheik-Bahae, Mansoor] Univ New Mexico, Dept Phys & Astron, Albuquerque, NM 87131 USA. [Cederberg, Jeffrey G.] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Yang, Z (reprint author), Univ New Mexico, Dept Phys & Astron, Albuquerque, NM 87131 USA. EM msb@unm.edu NR 10 TC 5 Z9 5 U1 1 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 978-1-62841-439-4 J9 PROC SPIE PY 2015 VL 9349 AR 934905 DI 10.1117/12.2079696 PG 6 WC Engineering, Electrical & Electronic; Optics; Physics, Applied SC Engineering; Optics; Physics GA BC5AN UT WOS:000353134900004 ER PT S AU Bilki, B AF Bilki, B. CA CALICE Collaboration GP IOP TI The CALICE digital hadron calorimeter: calibration and response to pions and positrons SO 16TH INTERNATIONAL CONFERENCE ON CALORIMETRY IN HIGH ENERGY PHYSICS (CALOR 2014) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 16th International Conference on Calorimetry in High Energy Physics (CALOR) CY APR 06-11, 2014 CL Justus Liebig Univ, Sci Campus, Giessen, GERMANY SP HIC FAIR Helmholtz Int Ctr HO Justus Liebig Univ, Sci Campus AB In order to measure the jet products of the hadronic decays of electroweak bosons in a future lepton collider with 3-4% resolution, a novel approach named Particle Flow Algorithms is proposed. The Particle Flow Algorithms attempt to measure each particle in a hadronic jet individually, using the detector providing the best energy/momentum resolution. The role of the hadronic calorimeters is to measure the neutral component of the hadronic jets. In this context, the CALICE Collaboration developed the Digital Hadron Calorimeter, which uses Resistive Plate Chambers as active media. The 1-bit resolution (digital) readout of 1 x 1 cm(2) pads achieves a world record in the number of readout channels already at the prototyping stage. Here we report on the results from the analysis of pion events of momenta between 2 to 60 GeV/c collected in the Fermi lab test beam with an emphasis on the intricate calibration procedures. C1 [Bilki, B.] Argonne Natl Lab, Argonne, IL 60439 USA. Univ Iowa, Iowa City, IA 52242 USA. RP Bilki, B (reprint author), Argonne Natl Lab, 9700 S Cass Ave, Argonne, IL 60439 USA. EM burak-bilki@uiowa.edu OI Bilki, Burak/0000-0001-9515-3306 NR 15 TC 0 Z9 0 U1 0 U2 1 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2015 VL 587 AR 012038 DI 10.1088/1742-6596/587/1/012038 PG 6 WC Physics, Particles & Fields SC Physics GA BC4CC UT WOS:000352292400038 ER PT S AU Bilki, B AF Bilki, B. CA CMS Collaboration GP IOP TI CMS Forward Calorimeters Phase II Upgrade SO 16TH INTERNATIONAL CONFERENCE ON CALORIMETRY IN HIGH ENERGY PHYSICS (CALOR 2014) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 16th International Conference on Calorimetry in High Energy Physics (CALOR) CY APR 06-11, 2014 CL Justus Liebig Univ, Sci Campus, Giessen, GERMANY SP HIC FAIR Helmholtz Int Ctr HO Justus Liebig Univ, Sci Campus ID PERFORMANCE; LHC; CALIBRATION; PARTICLE; DESIGN; WEDGES; BOSON AB The Phase II Upgrade of the CMS forward calorimeters (electromagnetic and hadronic) originates from the fact that these calorimeters will not be sufficiently performant with the expected HL-LHC (High Luminosity LHC) conditions. The major challenge is to preserve/improve the high performance of the current forward detectors with new devices that can withstand the unprecedented radiation levels and disentangle the very large event pileup. Here, we present an overview of the various upgrade options being considered by CMS, explaining the detector concepts and current/future beam test activities. C1 [Bilki, B.] Univ Iowa, Iowa City, IA 52242 USA. Argonne Natl Lab, Argonne, IL 60439 USA. RP Bilki, B (reprint author), Univ Iowa, Iowa City, IA 52242 USA. EM burak-bilki@uiowa.edu OI Bilki, Burak/0000-0001-9515-3306 NR 28 TC 3 Z9 3 U1 1 U2 3 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2015 VL 587 AR 012014 DI 10.1088/1742-6596/587/1/012014 PG 12 WC Physics, Particles & Fields SC Physics GA BC4CC UT WOS:000352292400014 ER PT S AU Bornheim, A Apresyan, A Duarte, J Pena, C Ronzhin, A Spiropulu, M Xie, S AF Bornheim, Adolf Apresyan, Artur Duarte, Javier Pena, Cristian Ronzhin, Anatoly Spiropulu, Maria Xie, Si GP IOP TI Calorimeters for Precision Timing Measurements in High Energy Physics SO 16TH INTERNATIONAL CONFERENCE ON CALORIMETRY IN HIGH ENERGY PHYSICS (CALOR 2014) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 16th International Conference on Calorimetry in High Energy Physics (CALOR) CY APR 06-11, 2014 CL Justus Liebig Univ, Sci Campus, Giessen, GERMANY SP HIC FAIR Helmholtz Int Ctr HO Justus Liebig Univ, Sci Campus AB Current and future high energy physics particle colliders are capable to provide instantaneous luminosities of 1034 cm-2s-1 and above. The high center of mass energy, the large number of simultaneous collision of beam particles in the experiments and the very high repetition rates of the collision events pose huge challenges. They result in extremely high particle fluxes, causing very high occupancies in the particle physics detectors operating at these machines. To reconstruct the physics events, the detectors have to make as much information as possible available on the final state particles. We discuss how timing information with a precision of around 10 ps and below can aid the reconstruction of the physics events under such challenging conditions. High energy photons play a crucial role in this context. About one third of the particle flux originating from high energy hadron collisions is detected as photons, stemming from the decays of neutral mesons. In addition, many key physics signatures under study are identified by high energy photons in the final state. They pose a particular challenge in that they can only be detected once they convert in the detector material. The particular challenge in measuring the time of arrival of a high energy photon lies in the stochastic component of the distance to the initial conversion and the size of the electromagnetic shower. They extend spatially over distances which propagation times of the initial photon and the subsequent electromagnetic shower which are large compared to the desired precision. We present studies and measurements from test beams and a cosmic muon test stand for calorimeter based timing measurements to explore the ultimate timing precision achievable for high energy photons of 10 GeV and above. We put particular focus on techniques to measure the timing with a precision of about 10 ps in association with the energy of the photon. For calorimeters utilizing scintillating materials and light guiding components, the propagation speed of the scintillation light in the calorimeter is important. We present studies and measurements of the propagation speed on a range of detector geometries. Finally, possible applications of precision timing in future high energy physics experiments are discussed. C1 [Bornheim, Adolf; Apresyan, Artur; Duarte, Javier; Pena, Cristian; Spiropulu, Maria; Xie, Si] CALTECH, Pasadena, CA 91125 USA. [Ronzhin, Anatoly] Fermilab Natl Accelerator Lab, Batavia, IL 60510 USA. RP Bornheim, A (reprint author), CALTECH, 1200 E Calif Blvd, Pasadena, CA 91125 USA. EM bornheim@hep.caltech.edu NR 3 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 2015 VL 587 AR 012057 DI 10.1088/1742-6596/587/1/012057 PG 11 WC Physics, Particles & Fields SC Physics GA BC4CC UT WOS:000352292400057 ER PT S AU Gatto, C Di Benedetto, V Mazzacane, A AF Gatto, C. Di Benedetto, V. Mazzacane, A. CA T1015 Collaboration GP IOP TI Status of ADRIANO R&D in T1015 Collaboration SO 16TH INTERNATIONAL CONFERENCE ON CALORIMETRY IN HIGH ENERGY PHYSICS (CALOR 2014) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 16th International Conference on Calorimetry in High Energy Physics (CALOR) CY APR 06-11, 2014 CL Justus Liebig Univ, Sci Campus, Giessen, GERMANY SP HIC FAIR Helmholtz Int Ctr HO Justus Liebig Univ, Sci Campus AB The physics program for future High Energy and High Intensity experiments requires an energy resolution of the calorimetric component of detectors at limits of traditional techniques and an excellent particle identification. The novel ADRIANO technology (A Dualreadout Integrally Active Non-segmented Option), currently under development at Fermilab, is showing excellent performance on those respects. Results from detailed Monte Carlo studies on the performance with respect to energy resolution, linear response and transverse containment and a preliminary optimization of the layout are presented. A baseline configuration is chosen with an estimated energy resolution of sigma(E)/E 30%/ root E, to support an extensive R&D program recently started by T1015 Collaboration at Fermilab. Preliminary results from several test beams at the Fermilab Test Beam Facility (FTBF) of a similar to 1 lambda 1 prototype are presented. Future prospects with ultra-heavy glass are, also, summarized. C1 [Gatto, C.; T1015 Collaboration] Ist Nazl Fis Nucl, Sez Napoli, I-80126 Naples, Italy. [Di Benedetto, V.; Mazzacane, A.] Fermilab Natl Accelerator Lab, Batavia, IL USA. RP Gatto, C (reprint author), Ist Nazl Fis Nucl, Sez Napoli, Via Cinthia, I-80126 Naples, Italy. EM corrado.gatto@na.infn.it NR 2 TC 0 Z9 0 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 2015 VL 587 AR 012060 DI 10.1088/1742-6596/587/1/012060 PG 9 WC Physics, Particles & Fields SC Physics GA BC4CC UT WOS:000352292400060 ER PT S AU Ma, H AF Ma, Hong CA ATLAS Liquid Argon Calorimeter Grp GP IOP TI Upgraded Trigger Readout Electronics for the ATLAS LAr Calorimeters for Future LHC Running SO 16TH INTERNATIONAL CONFERENCE ON CALORIMETRY IN HIGH ENERGY PHYSICS (CALOR 2014) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 16th International Conference on Calorimetry in High Energy Physics (CALOR) CY APR 06-11, 2014 CL Justus Liebig Univ, Sci Campus, Giessen, GERMANY SP HIC FAIR Helmholtz Int Ctr HO Justus Liebig Univ, Sci Campus AB The ATLAS Liquid Argon (LAr) calorimeters produce almost 200K signals that are digitized and processed by the front-end and back-end electronics for every triggered event. Additionally, the front-end electronics sums analog signals to provide coarse-grained energy sums to the first-level (L1) trigger system. The current design was optimized for the nominal LHC luminosity of 10(34)cm(-2)s(-1). In order to retain the capability to trigger on low energy electrons and photons when the LHC is upgraded to higher luminosity, an improved LAr calorimeter trigger readout is proposed and being constructed. The new trigger readout system makes available the fine segmentation of the calorimeter at the L1 trigger with high precision in order to reduce the QCD jet background in electron, photon and tau triggers, and to improve jet and missing ET trigger performance. The new LAr Trigger Digitizer Board is designed to receive the higher granularity signals, digitize them on-detector and send them via fast optical links to a new Digital Processing System. The reconstructed energies of trigger readout channels after digital filtering are transmitted to the L1 system, allowing the extraction of improved trigger signatures. This contribution presents the motivation for the upgrade, the concept for the new trigger readout and the expected performance of the new trigger, and describes the components being developed for the new system. C1 [Ma, Hong; ATLAS Liquid Argon Calorimeter Grp] Brookhaven Natl Lab, Dept Phys, Upton, NY 11973 USA. RP Ma, H (reprint author), Brookhaven Natl Lab, Dept Phys, Upton, NY 11973 USA. EM hina@bnl.gov RI Fabbri, Laura/H-3442-2012 OI Fabbri, Laura/0000-0002-4002-8353 NR 3 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 2015 VL 587 AR 012019 DI 10.1088/1742-6596/587/1/012019 PG 6 WC Physics, Particles & Fields SC Physics GA BC4CC UT WOS:000352292400019 ER PT S AU Pezzullo, G Budagov, J Carosi, R Cervelli, F Cheng, C Cordelli, M Corradi, G Davydov, Y Echenard, B Giovannella, S Glagolev, V Happacher, F Hitlin, D Luca, A Martini, M Miscetti, S Murat, P Ongmonkolkul, P Porter, F Saputi, A Sarra, I Spinella, F Stomaci, V Tassielli, G AF Pezzullo, Gianantonio Budagov, J. Carosi, R. Cervelli, F. Cheng, C. Cordelli, M. Corradi, G. Davydov, Yu. Echenard, B. Giovannella, S. Glagolev, V. Happacher, F. Hitlin, D. Luca, A. Martini, M. Miscetti, S. Murat, P. Ongmonkolkul, P. Porter, F. Saputi, A. Sarra, I. Spinella, F. Stomaci, V. Tassielli, G. GP IOP TI Progress status for the Mu2e calorimeter system SO 16TH INTERNATIONAL CONFERENCE ON CALORIMETRY IN HIGH ENERGY PHYSICS (CALOR 2014) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 16th International Conference on Calorimetry in High Energy Physics (CALOR) CY APR 06-11, 2014 CL Justus Liebig Univ, Sci Campus, Giessen, GERMANY SP HIC FAIR Helmholtz Int Ctr HO Justus Liebig Univ, Sci Campus AB The Mu2e experiment at FNAL aims to measure the charged-lepton flavor violating neutrinoless conversion of a negative muon into an electron. The conversion results in a monochromatic electron with an energy slightly below the muon rest mass (104.97 MeV). The calorimeter should confirm that the candidates reconstructed by the extremely precise tracker system are indeed conversion electrons while performing a powerful i/e particle identification. Moreover, it should also provide a high level trigger for the experiment independently from the tracker system. The calorimeter should also be able to keep functionality in an environment where the background delivers a dose of 10 krad/year in the hottest area and to work in the presence of 1 T axial magnetic field. These requirements translate in the design of a calorimeter with large acceptance, good energy resolution 0(5%) and a reasonable position (time) resolution of similar to <1 cm (<0.5ns). The baseline version of the calorimeter is composed by two disks of inner (outer) radius of 351 (660) mm filled by 1860 hexagonal BaF2 crystals of 20 cm length. Each crystal is readout by two large area APD's. In this paper, we summarize the experimental tests done so far as well as the simulation studies in the Mu2e environment. C1 [Pezzullo, Gianantonio] Univ Pisa, Dept Phys, I-56100 Pisa, Italy. Ist Nazl Fis Nucl, Sez Pisa, Pisa, Italy. Joint Inst Nucl Res, Dubna, Russia. CALTECH, Dept Phys, Pasadena, CA 91125 USA. Ist Nazl Fis Nucl, Lab Nazl Frascati, I-00044 Frascati, Italy. Ist Nazl Fis Nucl, Sez Lecce, I-73100 Lecce, Italy. Fermilab Natl Accelerator Lab, Batavia, IL 60510 USA. RP Pezzullo, G (reprint author), Univ Pisa, Dept Phys, Largo B Pontecorvo 3, I-56100 Pisa, Italy. EM pezzullo@pi.infn.it RI Tassielli, Giovanni Francesco/K-2929-2015; OI Tassielli, Giovanni Francesco/0000-0003-3410-6754; Giovannella, Simona/0000-0002-6243-1215; Pezzullo, Gianantonio/0000-0002-6653-1555 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 2015 VL 587 AR 012047 DI 10.1088/1742-6596/587/1/012047 PG 13 WC Physics, Particles & Fields SC Physics GA BC4CC UT WOS:000352292400047 ER PT S AU Ronzhin, A Los, S Ramberg, E Spiropulu, M Apresyan, A Xie, S Kim, H Zatserklyaniy, A AF Ronzhin, A. Los, S. Ramberg, E. Spiropulu, M. Apresyan, A. Xie, S. Kim, H. Zatserklyaniy, A. GP IOP TI New Fast Shower Max Detector Based on MCP as an Active Element SO 16TH INTERNATIONAL CONFERENCE ON CALORIMETRY IN HIGH ENERGY PHYSICS (CALOR 2014) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 16th International Conference on Calorimetry in High Energy Physics (CALOR) CY APR 06-11, 2014 CL Justus Liebig Univ, Sci Campus, Giessen, GERMANY SP HIC FAIR Helmholtz Int Ctr HO Justus Liebig Univ, Sci Campus AB One possibility to make a fast and radiation resistant shower maximum (SM) detector is to use a secondary emitter as an active element. We present below test beam results, obtained with different types of photo detectors based on micro channel plates (MCP) as secondary emitter. The SM time resolution - we obtained for this new type of detector is at the level of 20-30 ps. We estimate that a significant contribution to the detector response originates from secondary emission of the MCP. C1 [Ronzhin, A.; Los, S.; Ramberg, E.] Fermilab Natl Accelerator Lab, Batavia, IL 60510 USA. [Spiropulu, M.; Apresyan, A.; Xie, S.] CALTECH, Pasadena, CA 91125 USA. [Kim, H.] Univ Chicago, Chicago, IL 60637 USA. [Zatserklyaniy, A.] Univ Calif Santa Cruz, Santa Cruz, CA 95064 USA. RP Ronzhin, A (reprint author), Fermilab Natl Accelerator Lab, Batavia, IL 60510 USA. EM Artur.Apresyan@cern.ch NR 5 TC 0 Z9 0 U1 0 U2 0 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2015 VL 587 AR 012058 DI 10.1088/1742-6596/587/1/012058 PG 6 WC Physics, Particles & Fields SC Physics GA BC4CC UT WOS:000352292400058 ER PT S AU Seabra, L Alves, R Andringa, S Bradbury, S Carvalho, J Clark, K Coulter, I Descamps, F Falk, L Gurriana, L Kraus, C Lefeuvre, G Maio, A Maneira, J Mottram, M Peeters, S Rose, J Sinclair, J Skensved, P Waterfield, J White, R Wilson, J AF Seabra, L. Alves, R. Andringa, S. Bradbury, S. Carvalho, J. Clark, K. Coulter, I. Descamps, F. Falk, L. Gurriana, L. Kraus, C. Lefeuvre, G. Maio, A. Maneira, J. Mottram, M. Peeters, S. Rose, J. Sinclair, J. Skensved, P. Waterfield, J. White, R. Wilson, J. CA SNO Collaboration GP IOP TI The LED and fiber based calibration system for the photomultiplier array of SNO SO 16TH INTERNATIONAL CONFERENCE ON CALORIMETRY IN HIGH ENERGY PHYSICS (CALOR 2014) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 16th International Conference on Calorimetry in High Energy Physics (CALOR) CY APR 06-11, 2014 CL Justus Liebig Univ, Sci Campus, Giessen, GERMANY SP HIC FAIR Helmholtz Int Ctr HO Justus Liebig Univ, Sci Campus AB A new external LED/fiber light injection calibration system was designed for the calibration and monitoring of the photomultiplier array of the SNO+ experiment at SNOLAB. The goal of the calibration system is to allow an accurate and regular measurement of the photomultiplier array's performance, while minimizing the risk of radioactivity ingress. The choice in SNO+ was to use a set of optical fiber cables to convey into the detector the light pulses produced by external LEDs. The quality control was carried out using a modified test bench that was used in QC of optical fibers for TileCal/ATLAS. The optical fibers were characterized for transmission, timing and angular dispersions. This article describes the setups used for the characterization and quality control of the system based on LEDs and optical fibers and their results. C1 [Seabra, L.; Andringa, S.; Gurriana, L.; Maio, A.; Maneira, J.] Lab Instrumentacao & Fis Expt Particulas LIP, P-1000149 Lisbon, Portugal. [Alves, R.; Carvalho, J.] Univ Coimbra, Lab Instrumentacao & Fis Expt Particulas, P-3004516 Coimbra, Portugal. [Alves, R.; Carvalho, J.] Univ Coimbra, Dept Fis, P-3004516 Coimbra, Portugal. [Bradbury, S.] Univ Leeds, Sch Phys & Astron, Leeds LS2 9JT, W Yorkshire, England. [Clark, K.; Falk, L.; Lefeuvre, G.; Mottram, M.; Peeters, S.; Sinclair, J.; Waterfield, J.; White, R.] Univ Sussex, Dept Phys & Astron, Brighton BN1 9QH, E Sussex, England. [Coulter, I.] Univ Oxford, Dept Phys, Oxford OX1 3RH, England. [Descamps, F.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Nucl Sci, Berkeley, CA 94720 USA. [Kraus, C.] Laurentian Univ, Dept Phys & Astron, Sudbury, ON P3E 2C6, Canada. [Maio, A.; Maneira, J.] Univ Lisbon, Dept Fis, Fac Ciencias, P-1749016 Lisbon, Portugal. [Rose, J.] Univ Liverpool, Dept Phys, Liverpool L69 7ZE, Merseyside, England. [Maio, A.] Univ Lisbon, Ctr Fis Nucl, P-1649003 Lisbon, Portugal. [Skensved, P.] Queens Univ, Dept Phys, Kingston, ON K7L 3N6, Canada. [Wilson, J.] Univ London, Sch Phys & Astron, Queen Mary, London E1 4NS, England. RP Seabra, L (reprint author), Lab Instrumentacao & Fis Expt Particulas LIP, Av Elias Garcia 14,1, P-1000149 Lisbon, Portugal. EM lseabra@lip.pt RI Carvalho, Joao/M-4060-2013 OI Carvalho, Joao/0000-0002-3015-7821 NR 5 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 2015 VL 587 AR 012031 DI 10.1088/1742-6596/587/1/012031 PG 5 WC Physics, Particles & Fields SC Physics GA BC4CC UT WOS:000352292400031 ER PT S AU Tsai, OD Aschenauer, E Christie, W Dunkelberger, LE Fazio, S Gagliardi, CA Heppelmann, S Huang, HZ Jacobs, WW Igo, G Kisilev, A Landry, K Liu, X Mondal, MM Pan, YX Sergeeva, M Shah, N Sichtermann, E Trentalange, S Visser, G Wissink, S AF Tsai, O. D. Aschenauer, E. Christie, W. Dunkelberger, L. E. Fazio, S. Gagliardi, C. A. Heppelmann, S. Huang, H. Z. Jacobs, W. W. Igo, G. Kisilev, A. Landry, K. Liu, X. Mondal, M. M. Pan, Y. X. Sergeeva, M. Shah, N. Sichtermann, E. Trentalange, S. Visser, G. Wissink, S. GP IOP TI Development of a forward calorimeter system for the STAR experiment. SO 16TH INTERNATIONAL CONFERENCE ON CALORIMETRY IN HIGH ENERGY PHYSICS (CALOR 2014) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 16th International Conference on Calorimetry in High Energy Physics (CALOR) CY APR 06-11, 2014 CL Justus Liebig Univ, Sci Campus, Giessen, GERMANY SP HIC FAIR Helmholtz Int Ctr HO Justus Liebig Univ, Sci Campus AB We present results of an R&D program to develop a forward calorimeter system (FCS) for the STAR experiment at the Relativistic Heavy Ion Collider at BNL. The FCS is a very compact, compensated, finely granulated, high resolution calorimeter system being developed for p+p and p+A program at RHIC. The FCS prototype consists of both electromagnetic and hadron calorimeters. The electromagnetic portion of the detector is constructed with W powder and scintillation fibers. The hadronic calorimeter is a traditional Pb/Sc-plate sandwich design. Both calorimeters were readout with Hamamatsu MPPCs. A full-scale prototype of the FCS was tested with a beam at FNAL in March 2014. We present details of the design, construction technique and performance of the FCS prototype during the test run at FNAL. C1 [Tsai, O. D.; Dunkelberger, L. E.; Huang, H. Z.; Igo, G.; Landry, K.; Liu, X.; Pan, Y. X.; Sergeeva, M.; Shah, N.; Trentalange, S.] Univ Calif Los Angeles, Los Angeles, CA 90095 USA. [Aschenauer, E.; Christie, W.; Fazio, S.; Kisilev, A.] Brookhaven Natl Lab, Upton, NY 11973 USA. [Gagliardi, C. A.; Mondal, M. M.] Texas A&M Univ, College Stn, TX 77843 USA. [Heppelmann, S.] Penn State Univ, University Pk, PA 16802 USA. [Jacobs, W. W.; Visser, G.; Wissink, S.] Indiana Univ, CEEM, Bloomington, IN 47408 USA. [Sichtermann, E.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Tsai, OD (reprint author), Univ Calif Los Angeles, Los Angeles, CA 90095 USA. EM tsai@physics.ucla.edu RI Fazio, Salvatore /G-5156-2010 NR 4 TC 1 Z9 1 U1 0 U2 2 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2015 VL 587 AR 012053 DI 10.1088/1742-6596/587/1/012053 PG 10 WC Physics, Particles & Fields SC Physics GA BC4CC UT WOS:000352292400053 ER PT S AU Woody, C Kistenev, E AF Woody, C. Kistenev, E. CA PHENIX Collaboration GP IOP TI Design Studies of the Calorimeter Systems for the sPHENIX Experiment at RHIC and Future Upgrade Plans SO 16TH INTERNATIONAL CONFERENCE ON CALORIMETRY IN HIGH ENERGY PHYSICS (CALOR 2014) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 16th International Conference on Calorimetry in High Energy Physics (CALOR) CY APR 06-11, 2014 CL Justus Liebig Univ, Sci Campus, Giessen, GERMANY SP HIC FAIR Helmholtz Int Ctr HO Justus Liebig Univ, Sci Campus AB The PHENIX Experiment at RHIC is planning a series of major upgrades that will enable a comprehensive measurement of jets in relativistic heavy ion collisions, provide enhanced physics capabilities for studying nucleon-nucleus and polarized proton collisions, and allow a detailed study of electron-nucleus collisions at the Electron Ion Collider at Brookhaven (eRHIC). The first of these upgrades, sPHENIX, will be based on the former BaBar magnet and will include a hadronic calorimeter and new electromagnetic calorimeter that will cover 1.1 units in pseudorapidity and 27c in azimuth in the central region, resulting in a factor of 6 increase in acceptance over the present PHENIX detector. The electromagnetic calorimeter will be a tungsten scintillating fiber design with a radiation length 7 mm and a Moliere radius similar to 2 cm. It will have a total depth of 18 radiation lengths and an energy resolution 15%/4E. The hadronic calorimeter will consist of steel plates with scintillating tiles in between that are read out with wavelength shifting fibers, It will have a total depth of 5 interaction lengths and an energy resolution 100%/4E. Both calorimeters will use silicon photomultipliers as the readout sensor. Detailed design studies and Monte Carlo simulations for both calorimeters have been carried out and prototype detectors have been constructed and tested in a test beam at Fermi lab in February 2014. This contribution describes these design studies for the sPHENIX experiment and its future upgrade plans at RHIC. C1 [Woody, C.; Kistenev, E.] Brookhaven Natl Lab, Dept Phys, Upton, NY 11973 USA. RP Woody, C (reprint author), Brookhaven Natl Lab, Dept Phys, Bldg 510C, Upton, NY 11973 USA. EM woody@bnl.gov; kistenev@bnl.gov NR 3 TC 0 Z9 0 U1 0 U2 0 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2015 VL 587 AR 012054 DI 10.1088/1742-6596/587/1/012054 PG 8 WC Physics, Particles & Fields SC Physics GA BC4CC UT WOS:000352292400054 ER PT S AU Haranczyk, M Martin, RL AF Haranczyk, M. Martin, R. L. BE Vagenas, EC Vlachos, DS Bastos, C Hofer, T Kominis, Y Kosmas, O LeLay, G DePadova, P Rode, B Suraud, E Varga, K TI Mathematical Tools for Discovery of Nanoporous Materials for Energy Applications SO 3RD INTERNATIONAL CONFERENCE ON MATHEMATICAL MODELING IN PHYSICAL SCIENCES (IC-MSQUARE 2014) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 3rd International Conference on Mathematical Modeling in Physical Sciences (IC-MSQUARE) CY AUG 28-31, 2014 CL Madrid, SPAIN ID CRYSTALLINE POROUS MATERIALS; METAL-ORGANIC FRAMEWORKS; HIGH-SURFACE-AREA; POLYMER NETWORKS AB Porous materials such as zeolites and metal organic frameworks have been of growing importance as materials for energy-related applications such as CO2 capture, hydrogen and methane storage, and catalysis. The current state-of-the-art molecular simulations allow for accurate in silico prediction of materials' properties but the computational cost of such calculations prohibits their application in the characterisation of very large sets of structures, which would be required to perform brute-force screening. Our work focuses on the development of novel methodologies to efficiently characterize and explore this complex materials space. In particular, we have been developing algorithms and tools for enumeration and characterisation of porous material databases as well as efficient screening approaches. Our methodology represents a ensemble of mathematical methods. We have used Voronoi tessellation-based techniques to enable high-throughput structure characterisation, statistical techniques to perform comparison and screening, and continuous optimisation to design materials. This article outlines our developments in material design. C1 [Haranczyk, M.; Martin, R. L.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Haranczyk, M (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. EM mharanczyk@lbl.gov RI Haranczyk, Maciej/A-6380-2014 OI Haranczyk, Maciej/0000-0001-7146-9568 NR 14 TC 1 Z9 1 U1 1 U2 9 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2015 VL 574 AR 012103 DI 10.1088/1742-6596/574/1/012103 PG 5 WC Mathematics, Applied; Physics, Applied; Physics, Multidisciplinary SC Mathematics; Physics GA BC4LF UT WOS:000352595600103 ER PT S AU David, G AF David, Gabor GP IOP TI Event characterization in (very) asymmetric collisions SO 9TH INTERNATIONAL WORKSHOP ON HIGH-PT PHYSICS AT LHC SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 9th International Workshop on High-pT Physics at LHC CY SEP 24-28, 2013 CL Grenoble, FRANCE AB Event-by-event reconstruction of the collision geometry using some incarnation of the Glauber-model is a widely accepted method in studying heavy ion collisions. While there is no known problem with the procedure when applied to the collision of two large ions, we will argue that in very asymmetric collisions, like p(d)+A with at least one hard scattering process occuring the event geometry deduced with the simple Glauber-model may be biased. C1 Brookhaven Natl Lab, Upton, NY 11973 USA. RP David, G (reprint author), Brookhaven Natl Lab, Upton, NY 11973 USA. EM david@bnl.gov NR 12 TC 0 Z9 0 U1 1 U2 2 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2015 VL 589 AR 012005 DI 10.1088/1742-6596/589/1/012005 PG 6 WC Physics, Nuclear SC Physics GA BC4AG UT WOS:000352195100005 ER PT S AU Tannenbaum, MJ AF Tannenbaum, M. J. GP IOP TI How do quarks and gluons lose energy in the QGP? SO 9TH INTERNATIONAL WORKSHOP ON HIGH-PT PHYSICS AT LHC SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 9th International Workshop on High-pT Physics at LHC CY SEP 24-28, 2013 CL Grenoble, FRANCE ID LARGE TRANSVERSE-MOMENTUM; ROOT-S(NN)=2.76 TEV; INCLUSIVE PROCESSES; COLLISIONS; PHENIX; QCD AB RHIC introduced the method of hard scattering of partons as an in-situ probe of the the medium produced in A+A collisions. A suppression, R-AA approximate to 0.2 relative to binary-scaling, was discovered for pi(0) production in the range 5 <= p(T) <= 20 GeV/c in central Au+Au collisions at root s(NN) = 200 GeV, and surprisingly also for single-electrons from the decay of heavy quarks. Both these results have been confirmed in Pb+Pb collisions at the LHC at root s(NN) = 2.76 TeV. Interestingly, in this p(T) range the LHC results for pions nearly overlap the RHIC results. Thus, due to the flatter spectrum, the energy loss in the medium at LHC in this p(T) range must be similar to 40% larger than at RHIC. Unique at the LHC are the beautiful measurements of the fractional transverse momentum imbalance 1 - <(p) over capT(2)/(p) over capT(1)> of di-jets in Pb+Pb collisions. At the Utrecht meeting in 2011, I corrected for the fractional imbalance of di-jets with the same cuts in p-p collisions and showed that the relative fractional jet imbalance in Pb+Pb/p-p is approximate to 15% for jets with 120 <= (p) over capT(1)<= 360 GeV/c. CMS later confirmed this much smaller imbalance compared to the same quantity derived from two-particle correlations of di-jet fragments at RHIC corresponding to jet (p) over cap (T) approximate to 10-20 GeV/c, which appear to show a much larger fractional jet imbalance approximate to 45% in this lower (p) over cap (T) range. The variation of apparent energy loss in the medium as a function of both p(T) and root S-NN is striking and presents a challenge to both theory and experiment for improved understanding. There are many other such unresolved issues, for instance, the absence of evidence for (q) over cap effect, due to momentum transferred to the medium by outgoing partons, which would widen the away-side di-jet and di-hadron correlations in a similar fashion as the k(T)-effect. Another issue well known from experiments at the CERN ISR, SpS and SpS collider is that parton-parton hard-collisions make negligible contribution to multiplicity or transverse energy production in p-p collisions-soft particles, with p(T) <= 2 GeV/c, predominate. Thus an apparent hard scattering component for A+A multiplicity distributions based on a popular formula, dN(ch)(AA)/d eta = [(1 - x) < N-part > dN(ch)(pp)/d eta/2 + x < N-coll > dN(ch)(pp)/d eta], seems to be an unphysical way to understand the deviation from N-part scaling. Based on recent p-p and d+A measurements, a more physical way is presented along with several other stimulating results and ideas from recent d+Au (p+Pb) measurements. C1 Brookhaven Natl Lab, Dept Phys, Upton, NY 11973 USA. RP Tannenbaum, MJ (reprint author), Brookhaven Natl Lab, Dept Phys, Upton, NY 11973 USA. EM mjt@bnl.gov OI Tannenbaum, Michael/0000-0002-8840-5314 NR 54 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 2015 VL 589 AR 012019 DI 10.1088/1742-6596/589/1/012019 PG 16 WC Physics, Nuclear SC Physics GA BC4AG UT WOS:000352195100019 ER PT J AU Aalseth, CE Agnes, P Alton, A Arisaka, K Asner, DM Back, HO Baldin, B Biery, K Bonfini, G Bossa, M Brigatti, A Brodsky, J Budano, F Cadonati, L Cadoni, M Calaprice, F Canci, N Candela, A Cao, H Cariello, M Cavalcante, P Chepurnov, A Cocco, AG Condon, C Crippa, L D'Angelo, D D'Incecco, M Davini, S De Deo, M Derbin, A Devoto, A Di Eusanio, F Edkins, E Empl, A Fan, A Fiorillo, G Fomenko, K Forster, G Foxe, M Franco, D Gabriele, F Galbiati, C Goretti, A Grandi, L Gromov, M Guan, MY Guardincerri, Y Hackett, B Herner, K Hime, A Humble, P Hungerford, E Ianni, A Ianni, A Jaffe, DE Jollet, C Keeter, K Kendziora, C Kidner, S Kobychev, V Koh, G Korablev, D Korga, G Kurlej, A Li, PX Lissia, M Lombardi, P Ludhova, L Luitz, S Lukyachenko, G Ma, YQ Machulin, I Mandarano, A Mari, SM Maricic, J Marini, L Markov, D Martoff, J Meregaglia, A Meroni, E Meyers, PD Miletic, T Milincic, R Montuschi, M Monzani, ME Mosteiro, P Mount, B Muratova, V Musico, P Montanari, D Nelson, A Odrowski, S Odrzywolek, A Orrell, JL Orsini, M Ortica, F Pagani, L Pallavicini, M Pantic, E Parmeggiano, S Parsells, B Pelczar, K Pelliccia, N Perasso, S Perasso, L Pocar, A Pordes, S Pugachev, D Qian, H Randle, K Ranucci, G Razeto, A Recine, K Reinhold, B Renshaw, A Romani, A Rossi, N Rossi, B Rountree, SD Sablone, D Saggese, P Saldanha, R Sands, W Sangiorgio, S Segreto, E Semenov, D Shields, E Skorokhvatov, M Smallcomb, M Smirnov, O Sotnikov, A Suvurov, Y Tartaglia, R Tatarowicz, J Testera, G Tonazzo, A Unzhakov, E Vogelaar, RB Wada, M Walker, SE Wang, H Wang, Y Watson, AW Westerdale, S Williams, R Wojcik, M Xu, J Yang, CG Yoo, J Yu, B Zavatarelli, S Zhong, WL Zuzel, G AF Aalseth, C. E. Agnes, P. Alton, A. Arisaka, K. Asner, D. M. Back, H. O. Baldin, B. Biery, K. Bonfini, G. Bossa, M. Brigatti, A. Brodsky, J. Budano, F. Cadonati, L. Cadoni, M. Calaprice, F. Canci, N. Candela, A. Cao, H. Cariello, M. Cavalcante, P. Chepurnov, A. Cocco, A. G. Condon, C. Crippa, L. D'Angelo, D. D'Incecco, M. Davini, S. De Deo, M. Derbin, A. Devoto, A. Di Eusanio, F. Edkins, E. Empl, A. Fan, A. Fiorillo, G. Fomenko, K. Forster, G. Foxe, M. Franco, D. Gabriele, F. Galbiati, C. Goretti, A. Grandi, L. Gromov, M. Guan, M. Y. Guardincerri, Y. Hackett, B. Herner, K. Hime, A. Humble, P. Hungerford, E. Ianni, Al. Ianni, An. Jaffe, D. E. Jollet, C. Keeter, K. Kendziora, C. Kidner, S. Kobychev, V. Koh, G. Korablev, D. Korga, G. Kurlej, A. Li, P. X. Lissia, M. Lombardi, P. Ludhova, L. Luitz, S. Lukyachenko, G. Ma, Y. Q. Machulin, I. Mandarano, A. Mari, S. M. Maricic, J. Marini, L. Markov, D. Martoff, J. Meregaglia, A. Meroni, E. Meyers, P. D. Miletic, T. Milincic, R. Montuschi, M. Monzani, M. E. Mosteiro, P. Mount, B. Muratova, V. Musico, P. Montanari, D. Nelson, A. Odrowski, S. Odrzywolek, A. Orrell, J. L. Orsini, M. Ortica, F. Pagani, L. Pallavicini, M. Pantic, E. Parmeggiano, S. Parsells, B. Pelczar, K. Pelliccia, N. Perasso, S. Perasso, L. Pocar, A. Pordes, S. Pugachev, D. Qian, H. Randle, K. Ranucci, G. Razeto, A. Recine, K. Reinhold, B. Renshaw, A. Romani, A. Rossi, N. Rossi, B. Rountree, S. D. Sablone, D. Saggese, P. Saldanha, R. Sands, W. Sangiorgio, S. Segreto, E. Semenov, D. Shields, E. Skorokhvatov, M. Smallcomb, M. Smirnov, O. Sotnikov, A. Suvurov, Y. Tartaglia, R. Tatarowicz, J. Testera, G. Tonazzo, A. Unzhakov, E. Vogelaar, R. B. Wada, M. Walker, S. E. Wang, H. Wang, Y. Watson, A. W. Westerdale, S. Williams, R. Wojcik, M. Xu, J. Yang, C. G. Yoo, J. Yu, B. Zavatarelli, S. Zhong, W. L. Zuzel, G. TI The DarkSide Multiton Detector for the Direct Dark Matter Search SO ADVANCES IN HIGH ENERGY PHYSICS LA English DT Article ID GRAN SASSO; LIQUID ARGON AB Although the existence of dark matter is supported by many evidences, based on astrophysical measurements, its nature is still completely unknown. One major candidate is represented by weakly interacting massive particles (WIMPs), which could in principle be detected through their collisions with ordinary nuclei in a sensitive target, producing observable low-energy (< 100 keV) nuclear recoils. The DarkSide program aims at the WIPMs detection using a liquid argon time projection chamber (LAr-TPC). In this paper we quickly review the DarkSide program focusing in particular on the next generation experiment DarkSide-G2, a 3.6-ton LAr-TPC. The different detector components are described as well as the improvements needed to scale the detector from DarkSide50 (50 kg LAr-TPC) up to DarkSide-G2. Finally, the preliminary results on background suppression and expected sensitivity are presented. C1 [Aalseth, C. E.; Asner, D. M.; Foxe, M.; Hime, A.; Humble, P.; Orrell, J. L.; Williams, R.] Pacific NW Natl Lab, Richland, WA 99352 USA. [Agnes, P.; Franco, D.; Perasso, S.; Tonazzo, A.] Univ Paris Diderot, Sorbonne Paris Cite, APC, F-75205 Paris, France. [Alton, A.; Smallcomb, M.] Augustana Coll, Dept Phys & Astron, Sioux Falls, SD 57197 USA. [Arisaka, K.; Canci, N.; Fan, A.; Pantic, E.; Renshaw, A.; Suvurov, Y.; Wang, H.] Univ Calif Los Angeles, Dept Phys & Astron, Los Angeles, CA 90095 USA. [Back, H. O.; Brodsky, J.; Calaprice, F.; Cao, H.; Condon, C.; Di Eusanio, F.; Galbiati, C.; Goretti, A.; Ianni, An.; Koh, G.; Meyers, P. D.; Mosteiro, P.; Nelson, A.; Parsells, B.; Qian, H.; Rossi, B.; Sands, W.; Shields, E.; Wada, M.; Westerdale, S.; Xu, J.] Princeton Univ, Dept Phys, Princeton, NJ 08544 USA. [Baldin, B.; Biery, K.; Guardincerri, Y.; Herner, K.; Kendziora, C.; Montanari, D.; Pordes, S.; Yoo, J.] Fermilab Natl Accelerator Lab, Batavia, IL 60510 USA. [Bonfini, G.; Candela, A.; Cavalcante, P.; D'Incecco, M.; De Deo, M.; Gabriele, F.; Ianni, Al.; Montuschi, M.; Odrowski, S.; Orsini, M.; Razeto, A.; Rossi, N.; Segreto, E.; Tartaglia, R.] Lab Nazl Gran Sasso, I-67010 Assergi, Italy. [Bossa, M.] Gran Sasso Sci Inst, I-67100 Laquila, Italy. [Brigatti, A.; Crippa, L.; D'Angelo, D.; Lombardi, P.; Ludhova, L.; Meroni, E.; Parmeggiano, S.; Ranucci, G.; Saggese, P.] Univ Milan, Dept Phys, I-20133 Milan, Italy. [Brigatti, A.; Crippa, L.; D'Angelo, D.; Lombardi, P.; Ludhova, L.; Meroni, E.; Parmeggiano, S.; Ranucci, G.; Saggese, P.] Ist Nazl Fis Nucl, I-20133 Milan, Italy. [Budano, F.; Mandarano, A.; Mari, S. M.; Marini, L.] Univ Rome Tre, Dept Phys, I-00146 Rome, Italy. [Budano, F.; Mandarano, A.; Mari, S. M.; Marini, L.] Ist Nazl Fis Nucl, I-00146 Rome, Italy. [Cadonati, L.; Forster, G.; Kurlej, A.; Pocar, A.; Randle, K.] Univ Massachusetts, Dept Phys, Amherst, MA 01003 USA. [Cadoni, M.; Devoto, A.; Lissia, M.] Univ Cagliari, Dept Phys, I-09042 Cagliari, Italy. [Cadoni, M.; Devoto, A.; Lissia, M.] Ist Nazl Fis Nucl, I-09042 Cagliari, Italy. [Cariello, M.; Musico, P.; Pagani, L.; Pallavicini, M.; Perasso, L.; Testera, G.; Zavatarelli, S.] Univ Genoa, Dept Phys, I-16146 Genoa, Italy. [Cariello, M.; Musico, P.; Pagani, L.; Pallavicini, M.; Perasso, L.; Testera, G.; Zavatarelli, S.] Ist Nazl Fis Nucl, I-16146 Genoa, Italy. [Chepurnov, A.; Gromov, M.; Lukyachenko, G.] Moscow MV Lomonosov State Univ, Skobeltsyn Inst Nucl Phys, Moscow 119991, Russia. [Cocco, A. G.; Fiorillo, G.; Rossi, B.; Walker, S. E.] Univ Naples Federico II, Dept Phys, I-80126 Naples, Italy. [Cocco, A. G.; Fiorillo, G.; Rossi, B.; Walker, S. E.] Ist Nazl Fis Nucl, I-80126 Naples, Italy. [Davini, S.; Empl, A.; Hungerford, E.; Korga, G.; Sablone, D.] Univ Houston, Dept Phys, Houston, TX 77204 USA. [Derbin, A.; Muratova, V.; Semenov, D.; Unzhakov, E.] St Petersburg Nucl Phys Inst, Gatchina 188350, Russia. [Edkins, E.; Hackett, B.; Maricic, J.; Milincic, R.; Reinhold, B.] Univ Hawaii, Dept Phys & Astron, Honolulu, HI 96822 USA. [Fomenko, K.; Korablev, D.; Smirnov, O.; Sotnikov, A.] Joint Inst Nucl Res, Dubna 141980, Russia. [Grandi, L.; Saldanha, R.] Univ Chicago, Enrico Fermi Inst, Kavli Inst, Chicago, IL 60637 USA. [Grandi, L.; Saldanha, R.] Univ Chicago, Dept Phys, Chicago, IL 60637 USA. [Guan, M. Y.; Li, P. X.; Ma, Y. Q.; Wang, Y.; Yang, C. G.; Zhong, W. L.] Inst High Energy Phys, Beijing 100049, Peoples R China. [Jaffe, D. E.; Yu, B.] Brookhaven Natl Lab, Upton, NY 11973 USA. [Jollet, C.; Meregaglia, A.] Univ Strasbourg, CNRS, IN2P3, IPHC, F-67037 Strasbourg, France. [Keeter, K.; Mount, B.] Black Hills State Univ, Sch Nat Sci, Spearfish, SD 57799 USA. [Kidner, S.; Rountree, S. D.; Vogelaar, R. B.] Virginia Tech, Dept Phys, Blacksburg, VA 24061 USA. [Kobychev, V.] Natl Acad Sci Ukraine, Inst Nucl Res, UA-03680 Kiev, Ukraine. [Luitz, S.; Monzani, M. E.] SLAC Natl Accelerator Lab, Menlo Pk, CA 94025 USA. [Machulin, I.; Markov, D.; Pugachev, D.; Skorokhvatov, M.] Natl Res Ctr, Kurchatov Inst, Moscow 123182, Russia. [Martoff, J.; Miletic, T.; Recine, K.; Tatarowicz, J.; Watson, A. W.] Temple Univ, Dept Phys, Philadelphia, PA 19122 USA. [Odrzywolek, A.; Pelczar, K.; Wojcik, M.; Zuzel, G.] Jagiellonian Univ, Smoluchowski Inst Phys, PL-30059 Krakow, Poland. [Ortica, F.; Pelliccia, N.; Romani, A.] Univ Perugia, Dept Chem Biol & Biotechnol, I-06123 Perugia, Italy. [Ortica, F.; Pelliccia, N.; Romani, A.] Ist Nazl Fis Nucl, I-06123 Perugia, Italy. [Pantic, E.] Univ Calif Davis, Dept Phys, Davis, CA 95616 USA. [Sangiorgio, S.] Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. RP Fiorillo, G (reprint author), Univ Naples Federico II, Dept Phys, I-80126 Naples, Italy. EM giuliana.fiorillo@na.infn.it RI Yoo, Jonghee/K-8394-2016; Ortica, Fausto/C-1001-2013; Kobychev, Vladislav/B-3322-2008; DAngelo, Davide/K-9164-2013; Fiorillo, Giuliana/A-2248-2012; Romani, Aldo/G-8103-2012; Machulin, Igor/R-9711-2016; Skorokhvatov, Mikhail/R-9735-2016; Inst. of Physics, Gleb Wataghin/A-9780-2017; Razeto, Alessandro/J-3320-2015; Pallavicini, Marco/G-5500-2012; Humble, Paul/E-4766-2015; Humble, Paul/K-1961-2012; Orrell, John/E-9313-2015; Canci, Nicola/E-7498-2017; Ranucci, Gioacchino/O-2200-2015; OI Ortica, Fausto/0000-0001-8276-452X; Kobychev, Vladislav/0000-0003-0030-7451; DAngelo, Davide/0000-0001-9857-8107; Fiorillo, Giuliana/0000-0002-6916-6776; Romani, Aldo/0000-0002-7338-0097; Razeto, Alessandro/0000-0002-0578-097X; Pallavicini, Marco/0000-0001-7309-3023; Humble, Paul/0000-0002-2632-6557; Franco, Davide/0000-0001-5604-2531; Xu, Jingke/0000-0001-8084-5609; Unzhakov, Evgeniy/0000-0003-2952-6412; Westerdale, Shawn/0000-0001-8824-6205; Rossi, Nicola/0000-0002-7046-528X; Wang, Yi/0000-0002-7351-6978; Orrell, John/0000-0001-7968-4051; Canci, Nicola/0000-0002-4797-4297; Cadoni, Mariano/0000-0001-5595-7537; Rossi, Biagio/0000-0002-0807-8772; Devoto, Alberto/0000-0002-2263-734X; Ranucci, Gioacchino/0000-0002-3591-8191; Derbin, Alexander/0000-0002-4351-2255; Zhong, Weili/0000-0002-4566-5490 NR 38 TC 3 Z9 3 U1 6 U2 32 PU HINDAWI PUBLISHING CORP PI NEW YORK PA 410 PARK AVENUE, 15TH FLOOR, #287 PMB, NEW YORK, NY 10022 USA SN 1687-7357 EI 1687-7365 J9 ADV HIGH ENERGY PHYS JI Adv. High. Energy Phys. PY 2015 AR 541362 DI 10.1155/2015/541362 PG 8 WC Physics, Particles & Fields SC Physics GA CG2VL UT WOS:000353133400001 ER PT J AU Davies, CW Stjepanovic, G Hurley, JH AF Davies, Christopher W. Stjepanovic, Goran Hurley, James H. TI How the Atg1 complex assembles to initiate autophagy SO AUTOPHAGY LA English DT Editorial Material DE analytical ultracentrifugation; Atg13; Atg17; EAT domain; hydrogen-deuterium exchange mass spectrometry C1 [Davies, Christopher W.; Stjepanovic, Goran; Hurley, James H.] Univ Calif Berkeley, Dept Mol & Cell Biol, Berkeley, CA 94720 USA. [Davies, Christopher W.; Stjepanovic, Goran; Hurley, James H.] Univ Calif Berkeley, Calif Inst Quantitat Biosci, Berkeley, CA 94720 USA. [Hurley, James H.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Life Sci, Berkeley, CA 94720 USA. RP Hurley, JH (reprint author), Univ Calif Berkeley, Dept Mol & Cell Biol, 229 Stanley Hall, Berkeley, CA 94720 USA. EM jimhurley@berkeley.edu RI Stjepanovic, Goran/A-7902-2010 OI Stjepanovic, Goran/0000-0002-4841-9949 FU NIGMS NIH HHS [GM111730, F32 GM112301, GM112301, R01 GM111730] NR 0 TC 0 Z9 0 U1 0 U2 1 PU TAYLOR & FRANCIS INC PI PHILADELPHIA PA 530 WALNUT STREET, STE 850, PHILADELPHIA, PA 19106 USA SN 1554-8627 EI 1554-8635 J9 AUTOPHAGY JI Autophagy PD JAN PY 2015 VL 11 IS 1 BP 185 EP 186 DI 10.4161/15548627.2014.984281 PG 2 WC Cell Biology SC Cell Biology GA CF7ZA UT WOS:000352773700015 PM 25700739 ER PT J AU Porosoff, MD Kattel, S Li, WH Liu, P Chen, JG AF Porosoff, Marc D. Kattel, Shyam Li, Wenhui Liu, Ping Chen, Jingguang G. TI Identifying trends and descriptors for selective CO2 conversion to CO over transition metal carbides SO CHEMICAL COMMUNICATIONS LA English DT Article ID MOLYBDENUM CARBIDE; TUNGSTEN CARBIDE; CATALYSTS; HYDROGENATION; GAS; METHANE; ADSORPTION; SURFACES; ACTIVATION; REDUCTION AB Catalytic reduction of CO2 requires active, selective and low-cost catalysts. Results of this study show that transition metal carbides are a class of promising catalysts and their activity is correlated with oxygen binding energy and reducibility as shown by DFT calculations and in situ measurements. C1 [Porosoff, Marc D.; Li, Wenhui; Chen, Jingguang G.] Columbia Univ, Dept Chem Engn, New York, NY 10027 USA. [Kattel, Shyam; Liu, Ping; Chen, Jingguang G.] Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA. RP Chen, JG (reprint author), Columbia Univ, Dept Chem Engn, 500 W 120th St, New York, NY 10027 USA. EM jgchen@columbia.edu RI Porosoff, Marc/N-2816-2015 FU U.S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10886]; US Department of Energy; National Energy Research Scientific Computing Center (NERSC) - Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231] FX The work was carried out under Contract No. DE-AC02-98CH10886 with the U.S. Department of Energy, Office of Basic Energy Sciences. The DFT calculations were performed using computational resources at the Center for Functional Nanomaterials, BNL, supported by US Department of Energy and the National Energy Research Scientific Computing Center (NERSC) supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. NR 28 TC 11 Z9 12 U1 17 U2 103 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1359-7345 EI 1364-548X J9 CHEM COMMUN JI Chem. Commun. PY 2015 VL 51 IS 32 BP 6988 EP 6991 DI 10.1039/c5cc01545f PG 4 WC Chemistry, Multidisciplinary SC Chemistry GA CF5XM UT WOS:000352630600024 PM 25799361 ER PT J AU Trebotich, D Graves, DT AF Trebotich, David Graves, Daniel T. TI AN ADAPTIVE FINITE VOLUME METHOD FOR THE INCOMPRESSIBLE NAVIER-STOKES EQUATIONS IN COMPLEX GEOMETRIES SO COMMUNICATIONS IN APPLIED MATHEMATICS AND COMPUTATIONAL SCIENCE LA English DT Article DE incompressible Navier-Stokes; embedded boundary method; finite volume method; cut cell method; projection method; adaptive mesh refinement ID EMBEDDED BOUNDARY METHOD; HYPERBOLIC CONSERVATION-LAWS; CARTESIAN GRID METHOD; PROJECTION METHOD; EULER EQUATIONS; CYLINDER WAKE; IRREGULAR DOMAINS; MESH REFINEMENT; HEAT-EQUATION; VISCOUS-FLOW AB We present an adaptive, finite volume algorithm to solve the incompressible Navier-Stokes equations in complex geometries. The algorithm is based on the embedded boundary method, in which finite volume approximations are used to discretize the solution in cut cells that result from intersecting the irregular boundary with a structured Cartesian grid. This approach is conservative and reduces to a standard finite difference method in grid cells away from the boundary. We solve the incompressible flow equations using a predictor-corrector formulation. Hyperbolic advection terms are obtained by higher-order upwinding without the use of extrapolated data in covered cells. The small-cell stability problem associated with explicit embedded boundary methods for hyperbolic systems is avoided by the use of a volume-weighted scheme in the advection step and is consistent with construction of the right-hand side of the elliptic solvers. The Helmholtz equations resulting from viscous source terms are advanced in time by the Crank-Nicolson method, which reduces solver runtime compared to other second-order time integrators by a half. Incompressibility is enforced by a second-order approximate projection method that makes use of a new conservative cell-centered gradient in cut cells that is consistent with the volume-weighted scheme. The algorithm is also capable of block structured adaptive mesh refinement to increase spatial resolution dynamically in regions of interest. The resulting overall method is second-order accurate for sufficiently smooth problems. In addition, the algorithm is implemented in a high-performance computing framework and can perform structured-grid fluid dynamics calculations at unprecedented scale and resolution, up to 262,144 processor cores. We demonstrate robustness and performance of the algorithm by simulating incompressible flow for a wide range of Reynolds numbers in two and three dimensions: Stokes and low Reynolds number flows in both constructed and image data geometries (Re << 1 to Re = 1), flow past a cylinder (Re = 300), flow past a sphere (Re = 600) and turbulent flow in a contraction (Re = 6300). C1 [Trebotich, David; Graves, Daniel T.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Computat Res Div, Berkeley, CA 94720 USA. RP Trebotich, D (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Computat Res Div, 1 Cyclotron Rd, Berkeley, CA 94720 USA. EM dptrebotich@lbl.gov; dtgraves@lbl.gov FU U.S. Department of Energy, Office of Science, Office of Advanced Scientific Computing Research; Office of Basic Energy Sciences Energy Frontier Research Centers; National Energy Research Scientific Computing Center [DE-AC02-05CH11231]; Oak Ridge Leadership Computing Facility; Office of Science of the DOE [DE-AC05-00OR22725, DE-AC02-06CH11357]; Argonne National Laboratory; Office of Science, Office of Basic Energy Sciences, of the DOE [DE-AC02-05CH11231] FX This material is based upon work supported by the U.S. Department of Energy, Office of Science, Office of Advanced Scientific Computing Research and in part by the Office of Basic Energy Sciences Energy Frontier Research Centers and used resources of the National Energy Research Scientific Computing Center all under contract number DE-AC02-05CH11231. This research used resources of the Oak Ridge Leadership Computing Facility, which is a DOE Office of Science User Facility supported by the Office of Science of the DOE under contract number DE-AC05-00OR22725. This research used resources of the Argonne Leadership Computing Facility at Argonne National Laboratory, which is supported by the Office of Science of the DOE under contract DE-AC02-06CH11357. Simulation data in Figure 12 is based upon synchrotron microtomography imagery acquired by Jonathan Ajo-Franklin and Marco Voltolini at the Advanced Light Source, Beamline 8.3.2, which is supported by the Office of Science, Office of Basic Energy Sciences, of the DOE under contract DE-AC02-05CH11231. Simulation data in Figure 13 is based upon FIB-SEM imagery obtained by Lisa Chan at Tescan USA and processed by Terry Ligocki (LBNL), courtesy of Tim Kneafsey (LBNL). NR 59 TC 7 Z9 7 U1 2 U2 15 PU MATHEMATICAL SCIENCE PUBL PI BERKELEY PA UNIV CALIFORNIA, DEPT MATHEMATICS, BERKELEY, CA 94720-3840 USA SN 1559-3940 EI 2157-5452 J9 COMM APP MATH COM SC JI Commun. Appl. Math. Comput. Sci. PY 2015 VL 10 IS 1 BP 43 EP 82 DI 10.2140/camcos.2015.10.43 PG 40 WC Mathematics, Applied; Physics, Mathematical SC Mathematics; Physics GA CG0TG UT WOS:000352982000003 ER PT J AU Schwartz, P Percelay, J Ligocki, TJ Johansen, H Graves, DT Devendran, D Colella, P Ateljevich, E AF Schwartz, Peter Percelay, Julie Ligocki, Terry J. Johansen, Hans Graves, Daniel T. Devendran, Dharshi Colella, Phillip Ateljevich, Eli TI HIGH-ACCURACY EMBEDDED BOUNDARY GRID GENERATION USING THE DIVERGENCE THEOREM SO COMMUNICATIONS IN APPLIED MATHEMATICS AND COMPUTATIONAL SCIENCE LA English DT Article DE Cartesian grid embedded boundaries; grid generation; finite volume methods ID NAVIER-STOKES EQUATIONS; POISSONS-EQUATION; DIMENSIONS; MOMENTS; FLOW; 3D AB We present an algorithm to produce the necessary geometric information for finite volume calculations in the context of Cartesian grids with embedded boundaries. Given an order of accuracy for the overall calculation, we show what accuracy is required for each of the geometric quantities and we demonstrate how to calculate the moments using the divergence theorem. We demonstrate that, for a known flux, these moments can be used to create a flux divergence of the expected order. C1 [Schwartz, Peter; Ligocki, Terry J.; Johansen, Hans; Graves, Daniel T.; Devendran, Dharshi; Colella, Phillip] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Appl Numer Algorithms Grp, Berkeley, CA 94720 USA. [Percelay, Julie] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Ateljevich, Eli] Calif Dept Water Resources, Sacramento, CA 95821 USA. RP Schwartz, P (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Appl Numer Algorithms Grp, 1 Cyclotron Rd, Berkeley, CA 94720 USA. EM poschwartz@lbl.gov; julie.percelay@gmail.com; tjligocki@lbl.gov; hjohansen@lbl.gov; dtgraves@lbl.gov; pdevendran@lbl.gov; pcolella@lbl.gov; eli.ateljevich@water.ca.gov FU Office of Advanced Scientific Computing Research of the US Department of Energy [DE-AC02-05CH11231] FX Research at LBNL was supported financially by the Office of Advanced Scientific Computing Research of the US Department of Energy under contract number DE-AC02-05CH11231. All work was done using the Chombo software infrastructure developed by LBNL [4; 5]. NR 19 TC 1 Z9 1 U1 1 U2 3 PU MATHEMATICAL SCIENCE PUBL PI BERKELEY PA UNIV CALIFORNIA, DEPT MATHEMATICS, BERKELEY, CA 94720-3840 USA SN 1559-3940 EI 2157-5452 J9 COMM APP MATH COM SC JI Commun. Appl. Math. Comput. Sci. PY 2015 VL 10 IS 1 BP 83 EP 96 DI 10.2140/camcos.2015.10.83 PG 14 WC Mathematics, Applied; Physics, Mathematical SC Mathematics; Physics GA CG0TG UT WOS:000352982000004 ER PT J AU Azarbad, H Niklinska, M Laskowski, R van Straalen, NM van Gestel, CAM Zhou, JZ He, ZL Wen, CQ Roling, WFM AF Azarbad, Hamed Niklinska, Maria Laskowski, Ryszard van Straalen, Nico M. van Gestel, Cornelis A. M. Zhou, Jizhong He, Zhili Wen, Chongqing Roeling, Wilfred F. M. TI Microbial community composition and functions are resilient to metal pollution along two forest soil gradients SO FEMS MICROBIOLOGY ECOLOGY LA English DT Article DE Illumina sequencing; GeoChip; metal pollution; soil microbial communities ID HEAVY-METALS; BACTERIAL COMMUNITIES; DIVERSITY; MICROARRAY; CONTAMINATION; BIODIVERSITY; RESISTANCE; SEDIMENTS; GEOCHIP; LITTER AB Despite the global importance of forests, it is virtually unknown how their soil microbial communities adapt at the phylogenetic and functional level to long-term metal pollution. Studying 12 sites located along two distinct gradients of metal pollution in Southern Poland revealed that functional potential and diversity (assessed using GeoChip 4.2) were highly similar across the gradients despite drastically diverging metal contamination levels. Metal pollution level did, however, significantly impact bacterial community structure (as shown by MiSeq Illumina sequencing of 16S rRNA genes), but not bacterial taxon richness and community composition. Metal pollution caused changes in the relative abundance of specific bacterial taxa, including Acidobacteria, Actinobacteria, Bacteroidetes, Chloroflexi, Firmicutes, Planctomycetes and Proteobacteria. Also, a group of metal-resistance genes showed significant correlations with metal concentrations in soil. Our study showed that microbial communities are resilient to metal pollution; despite differences in community structure, no clear impact of metal pollution levels on overall functional diversity was observed. While screens of phylogenetic marker genes, such as 16S rRNA genes, provide only limited insight into resilience mechanisms, analysis of specific functional genes, e.g. involved in metal resistance, appears to be a more promising strategy. C1 [Azarbad, Hamed; Niklinska, Maria; Laskowski, Ryszard] Jagiellonian Univ, Inst Environm Sci, PL-30387 Krakow, Poland. [van Straalen, Nico M.; van Gestel, Cornelis A. M.] Vrije Univ Amsterdam, Fac Earth & Life Sci, Dept Ecol Sci, NL-1081 HV Amsterdam, Netherlands. [Zhou, Jizhong; He, Zhili; Wen, Chongqing] Univ Oklahoma, Inst Environm Genom, Norman, OK 73072 USA. [Zhou, Jizhong; He, Zhili; Wen, Chongqing] Univ Oklahoma, Dept Microbiol, Norman, OK 73072 USA. [Zhou, Jizhong; He, Zhili; Wen, Chongqing] Univ Oklahoma, Dept Plant Biol, Norman, OK 73072 USA. [Zhou, Jizhong] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. [Zhou, Jizhong] Tsinghua Univ, Sch Environm, State Key Joint Lab Environm Simulat & Pollut Con, Beijing 100084, Peoples R China. [Roeling, Wilfred F. M.] Vrije Univ Amsterdam, Dept Mol Cell Physiol, Fac Earth & Life Sci, NL-1081 HV Amsterdam, Netherlands. RP Azarbad, H (reprint author), Jagiellonian Univ, Inst Environm Sci, Gronostajowa 7, PL-30387 Krakow, Poland. EM Hamed.Azarbad@uj.edu.pl RI Laskowski, Ryszard/A-2680-2009; OI Laskowski, Ryszard/0000-0002-1968-3230; van Gestel, Kees/0000-0002-5651-0208 FU 'Environmental stress, population viability and adaptation' project [MPD/2009-3/5]; Institute of Environmental Sciences, Jagiellonian University [DS759] FX This study was performed within the 'Environmental stress, population viability and adaptation' project (No. MPD/2009-3/5) and supported by the DS759 of the Institute of Environmental Sciences, Jagiellonian University. NR 50 TC 13 Z9 14 U1 19 U2 99 PU OXFORD UNIV PRESS PI OXFORD PA GREAT CLARENDON ST, OXFORD OX2 6DP, ENGLAND SN 0168-6496 EI 1574-6941 J9 FEMS MICROBIOL ECOL JI FEMS Microbiol. Ecol. PD JAN PY 2015 VL 91 IS 1 DI 10.1093/femsec/fiu003 PG 11 WC Microbiology SC Microbiology GA CF8BT UT WOS:000352781000002 PM 25764529 ER PT J AU Mahmoudi, N Robeson, MS Castro, HF Fortney, JL Techtmann, SM Joyner, DC Paradis, CJ Pfiffner, SM Hazen, TC AF Mahmoudi, Nagissa Robeson, Michael S., II Castro, Hector F. Fortney, Julian L. Techtmann, Stephen M. Joyner, Dominique C. Paradis, Charles J. Pfiffner, Susan M. Hazen, Terry C. TI Microbial community composition and diversity in Caspian Sea sediments SO FEMS MICROBIOLOGY ECOLOGY LA English DT Article DE Caspian Sea; marine sediments; bacteria; archaea; Illumina; PLFA ID DEEP MARINE-SEDIMENTS; CONTINENTAL-MARGIN SEDIMENTS; AMMONIA-OXIDIZING ARCHAEA; SULFATE-REDUCING BACTERIA; METHANE TRANSITION ZONE; OIL-DEGRADING BACTERIA; EAST CHINA SEA; SUBSEAFLOOR SEDIMENTS; BENTHIC MACROFAUNA; ORGANIC-MATTER AB The Caspian Sea is heavily polluted due to industrial and agricultural effluents as well as extraction of oil and gas reserves. Microbial communities can influence the fate of contaminants and nutrients. However, insight into the microbial ecology of the Caspian Sea significantly lags behind other marine systems. Here we describe microbial biomass, diversity and composition in sediments collected from three sampling stations in the Caspian Sea. Illumina sequencing of 16S rRNA genes revealed the presence of a number of known bacterial and archaeal heterotrophs suggesting that organic carbon is a primary factor shaping microbial communities. Surface sediments collected from bottom waters with low oxygen levels were dominated by Gammaproteobacteria while surface sediments collected from bottom waters under hypoxic conditions were dominated by Deltaproteobacteria, specifically sulfate-reducing bacteria. Thaumarchaeota was dominant across all surface sediments indicating that nitrogen cycling in this system is strongly influenced by ammonia-oxidizing archaea. This study provides a baseline assessment that may serve as a point of reference as this system changes or as the efficacy of new remediation efforts are implemented. C1 [Mahmoudi, Nagissa; Fortney, Julian L.; Techtmann, Stephen M.; Joyner, Dominique C.; Hazen, Terry C.] Univ Tennessee, Dept Civil & Environm Engn, Knoxville, TN 37996 USA. [Robeson, Michael S., II; Hazen, Terry C.] Oak Ridge Natl Lab, BioSci Div, Oak Ridge, TN 37831 USA. [Castro, Hector F.] Univ Tennessee, Dept Chem, Knoxville, TN 37996 USA. [Mahmoudi, Nagissa; Fortney, Julian L.; Techtmann, Stephen M.; Joyner, Dominique C.; Pfiffner, Susan M.; Hazen, Terry C.] Univ Tennessee, Ctr Environm Biotechnol, Knoxville, TN 37996 USA. [Paradis, Charles J.; Hazen, Terry C.] Univ Tennessee, Dept Earth & Planetary Sci, Knoxville, TN 37996 USA. [Hazen, Terry C.] Univ Tennessee, Dept Microbiol, Knoxville, TN 37996 USA. RP Mahmoudi, N (reprint author), Univ Tennessee, Dept Civil & Environm Engn, 1414 Circle Dr, Knoxville, TN 37996 USA. EM nagissa.m@gmail.com RI Hazen, Terry/C-1076-2012; OI Hazen, Terry/0000-0002-2536-9993; Robeson, Michael/0000-0001-7119-6301 FU University of Tennessee [A13-0119-001]; BP America [A13-0119-001] FX This research was supported by contract A13-0119-001 Deep Sea Basin Microbiology between the University of Tennessee and BP America. NR 89 TC 5 Z9 5 U1 8 U2 52 PU OXFORD UNIV PRESS PI OXFORD PA GREAT CLARENDON ST, OXFORD OX2 6DP, ENGLAND SN 0168-6496 EI 1574-6941 J9 FEMS MICROBIOL ECOL JI FEMS Microbiol. Ecol. PD JAN PY 2015 VL 91 IS 1 DI 10.1093/femsec/fiu013 PG 11 WC Microbiology SC Microbiology GA CF8BT UT WOS:000352781000009 ER PT J AU Chen, B Shi, J Zheng, XJ Zhou, Y Zhu, K Priya, S AF Chen, Bo Shi, Jian Zheng, Xiaojia Zhou, Yuan Zhu, Kai Priya, Shashank TI Ferroelectric solar cells based on inorganic-organic hybrid perovskites SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID ORGANOMETAL HALIDE PEROVSKITES; HIGH-EFFICIENCY; PHOTOVOLTAIC DEVICES; IODIDE PEROVSKITES; CHARGE SEPARATION; THIN-FILMS; BAND-GAP; BIFEO3; ELECTRON; ENHANCEMENT AB Ferroelectric solar cells based on ferroelectric oxides have attracted significant attention owing to many unique advantages, such as the switchable photocurrent and photovoltage, and the above bandgap open circuit voltages. However, the small photocurrent densities of the typical ferroelectric solar cells greatly limit their photovoltaic performance. In this report, we experimentally revealed the polarization switching properties of inorganic-organic hybrid perovskites and developed ferroelectric solar cells based on the hybrid perovskites. Hybrid perovskite methylammonium lead trihalide (MAPbX(3)) thin films exhibited 180 degrees domain phase switching and polarization hysteresis loops. Ferroelectric solar cells based on the mixed halide MAPbI(3-x)Cl(x) thin film demonstrate a power conversion efficiency of 6.7% and the ferroelectric solar cells display switchable photovoltaic effects. This work provides an alternative but exhilarating solution for high-performance ferroelectric solar cells beyond inorganic ferroelectric oxides. C1 [Chen, Bo; Zheng, Xiaojia; Zhou, Yuan; Priya, Shashank] Virginia Tech, Ctr Energy Harvesting Mat & Syst, Blacksburg, VA 24061 USA. [Shi, Jian] Rensselaer Polytech Inst, Dept Mat Sci & Engn, Troy, NY 12180 USA. [Zhu, Kai] Natl Renewable Energy Lab, Chem & Nanosci Ctr, Golden, CO 80401 USA. RP Chen, B (reprint author), Virginia Tech, Ctr Energy Harvesting Mat & Syst, Blacksburg, VA 24061 USA. EM bochen09@vt.edu; xiaojia@vt.edu; spriya@vt.edu OI Zheng, Xiaojia/0000-0002-3963-4073 FU US Army [W15P7T-13-C-A910]; U.S. Department of Energy [DE-AC36-08-GO28308]; U.S. Department of Energy (DOE) SunShot Initiative under the Next Generation Photovoltaics 3 program [DE-FOA-0000990] FX The authors gratefully acknowledge the financial support through US Army under contract no. W15P7T-13-C-A910. The work at the National Renewable Energy Laboratory was supported by the U.S. Department of Energy under Contract no. DE-AC36-08-GO28308. K.Z. acknowledges the support by the U.S. Department of Energy (DOE) SunShot Initiative under the Next Generation Photovoltaics 3 program (DE-FOA-0000990). NR 64 TC 30 Z9 30 U1 13 U2 123 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7488 EI 2050-7496 J9 J MATER CHEM A JI J. Mater. Chem. A PY 2015 VL 3 IS 15 BP 7699 EP 7705 DI 10.1039/c5ta01325a PG 7 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA CF3IF UT WOS:000352441100003 ER PT J AU Wu, M Wang, J Wu, ZX Xin, HLL Wang, DL AF Wu, Min Wang, Jie Wu, Zexing Xin, Huolin L. Wang, Deli TI Synergistic enhancement of nitrogen and sulfur co-doped graphene with carbon nanosphere insertion for the electrocatalytic oxygen reduction reaction SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID METAL-FREE ELECTROCATALYSTS; ALKALINE-MEDIUM; NANOTUBES; CATALYST; BORON; OXIDE; MEDIA; PERFORMANCE AB A carbon black incorporated nitrogen and sulfur co-doped graphene (NSGCB) nanocomposite has been synthesized through one-pot annealing of a precursor mixture containing graphene oxide, thiourea, and acidized carbon black (CB). The NSGCB shows excellent performance for the oxygen reduction reaction (ORR) with the onset and half-wave potentials at 0.96 V and 0.81 V (vs. RHE), respectively, which are significantly higher compared to those of the catalysts derived from only graphene (0.90 V and 0.76 V) or carbon nanospheres (0.82 V and 0.74 V). The enhanced catalytic activity of the NSGCB electrode could be attributed to the synergistic effect of N/S co-doping and the enlarged interlayer space resulted from the insertion of carbon nanospheres into the graphene sheets. The four-electron selectivity and the limiting current density of the NSGCB nanocomposite are comparable to those of the commercial Pt/C catalyst. Furthermore, the NSGCB nanocomposite is superior to Pt/C in terms of long-term durability and tolerance to methanol poisoning. C1 [Wu, Min; Wang, Jie; Wu, Zexing; Wang, Deli] Huazhong Univ Sci & Technol, Key Lab Large Format Battery Mat & Syst, Minist Educ, Sch Chem & Chem Engn, Wuhan 430074, Peoples R China. [Xin, Huolin L.] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. [Xin, Huolin L.] SUNY Stony Brook, Dept Mat Sci & Engn, Stony Brook, NY 11794 USA. RP Wang, DL (reprint author), Huazhong Univ Sci & Technol, Key Lab Large Format Battery Mat & Syst, Minist Educ, Sch Chem & Chem Engn, Wuhan 430074, Peoples R China. EM wangdl81125@hust.edu.cn RI Wang, Deli/K-5029-2012; Wang, Jie/H-3638-2015; Xin, Huolin/E-2747-2010 OI Wang, Jie/0000-0002-7188-3053; Xin, Huolin/0000-0002-6521-868X FU National Science Foundation of China [21306060]; Program for New Century Excellent Talents in Universities of China [NCET-13-0237]; Doctoral Fund of Ministry of Education of China [20130142120039]; Fundamental Research Funds for the Central University [2013TS136, 2014YQ009]; U.S. Department of Energy, Office of Basic Energy Sciences [DE-SC0012704] FX This work was supported by the National Science Foundation of China (21306060), the Program for New Century Excellent Talents in Universities of China (NCET-13-0237), the Doctoral Fund of Ministry of Education of China (20130142120039), the Fundamental Research Funds for the Central University (2013TS136, 2014YQ009). This research carried out in part at the Center for Functional Nanomaterials, Brookhaven National Laboratory, which is supported by the U.S. Department of Energy, Office of Basic Energy Sciences, under Contract no. DE-SC0012704. We thank Analytical and Testing Center of Huazhong University of Science& Technology for allowing us to use its facilities. NR 33 TC 9 Z9 10 U1 13 U2 77 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7488 EI 2050-7496 J9 J MATER CHEM A JI J. Mater. Chem. A PY 2015 VL 3 IS 15 BP 7727 EP 7731 DI 10.1039/c4ta06323f PG 5 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA CF3IF UT WOS:000352441100008 ER PT J AU Lee, K Ruddy, DA Dukovic, G Neale, NR AF Lee, Kyureon Ruddy, Daniel A. Dukovic, Gordana Neale, Nathan R. TI Synthesis, optical, and photocatalytic properties of cobalt mixed-metal spinel oxides Co(Al1-xGax)(2)O-4 SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID SOL-GEL SYNTHESIS; ZERO CHARGE; HYDROGEN-PRODUCTION; QUANTUM DOTS; WATER; PHOTOELECTROLYSIS; NANOCRYSTALS; PHOTOANODES; PRECURSORS; POINTS AB Cobalt mixed-metal spinel oxides, Co(Al1-xGax)(2)O-4, have been predicted to exhibit promising properties as photocatalysts for solar energy conversion. In this work, Co(Al1-xGax)(2)O-4 were synthesized with a range of 0 <= x <= 1 via both single-source and multi-source routes. Single-source molecular precursors, [Co{M((OBu)-Bu-t)(4)}(2)] (M = Al or Ga), were decomposed at 300 degrees C to form amorphous oxides. Multi-source precursors, stoichiometric mixtures of metal acetylacetonate (acac) complexes, were used to form nanocrystalline spinel materials. Both were subsequently converted to bulk spinel products by annealing at 1000 degrees C. The properties of materials fabricated from the single-source and multi-source synthetic routes were compared by analysing data from X-ray diffraction, scanning electron microscopy, transmission electron microscopy, UV-vis spectrophotometry, inductively coupled plasma-optical emission spectroscopy, and gas sorption measurements. The X-ray diffraction data of the materials showed ideal solid solution behavior that followed Vegard's law for both routes, with the multi-source route giving more crystalline bulk material than the single-source route. UV-vis absorbance data revealed that the absorption onset energies of Co(Al1-xGax)(2)O-4 decreased monotonically with increasing x (from 1.84 eV for x = 0 to 1.76 eV for x = 1 from the single-source method; 1.75 eV for x = 0 to 1.70 eV for x = 1 from the multi-source method). The photocatalytic activities of the spinel oxides were evaluated via the photodegradation of methyl orange and phenol, which showed that the photoactivity of Co(Al0.5Ga0.5)(2)O-4 was dependent on both pH and substrate. Remarkably, under appropriate substrate binding conditions (pH 3 with methyl orange), low energy (<2.5 eV) ligand-field transitions contributed between 46 and 72% of the photoactivity of Co(Al0.5Ga0.5)(2)O-4 prepared from the multi-source route. C1 [Lee, Kyureon; Dukovic, Gordana] Univ Colorado, Dept Chem & Biochem, Boulder, CO 80309 USA. [Ruddy, Daniel A.; Neale, Nathan R.] Natl Renewable Energy Lab, Chem & Nanosci Ctr, Golden, CO 80401 USA. RP Dukovic, G (reprint author), Univ Colorado, Dept Chem & Biochem, Campus Box 215, Boulder, CO 80309 USA. EM Dan.Ruddy@nrel.gov; Gordana.Dukovic@colorado.edu; Nathan.Neale@nrel.gov FU NREL's Laboratory Directed Research and Development (LDRD) program; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences [DE-AC36-08GO28308] FX Molecular and material synthesis and characterization was funded by NREL's Laboratory Directed Research and Development (LDRD) program. Photocatalytic experimental design and data interpretation was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences through Contract no. DE-AC36-08GO28308 to NREL. NR 38 TC 7 Z9 7 U1 2 U2 14 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7488 EI 2050-7496 J9 J MATER CHEM A JI J. Mater. Chem. A PY 2015 VL 3 IS 15 BP 8115 EP 8122 DI 10.1039/c4ta06690a PG 8 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA CF3IF UT WOS:000352441100055 ER PT J AU Zhou, YY Yang, MJ Wu, WW Vasiliev, AL Zhu, K Padture, NP AF Zhou, Yuanyuan Yang, Mengjin Wu, Wenwen Vasiliev, Alexander L. Zhu, Kai Padture, Nitin P. TI Room-temperature crystallization of hybrid-perovskite thin films via solvent-solvent extraction for high-performance solar cells SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID ORGANOMETAL HALIDE PEROVSKITES; PLANAR HETEROJUNCTION; HOLE-CONDUCTOR; EFFICIENCY; IODIDE; DEPOSITION; EMERGENCE; LIGHT AB The room-temperature solvent-solvent extraction (SSE) concept is used for the deposition of hybrid-perovskite thin films over large areas. In this simple process, perovskite precursor solution is spin-coated onto a substrate, and instead of the conventional thermal annealing treatment, the coated substrate is immediately immersed in a bath of another solvent at room temperature. This results in efficient extraction of the precursor-solvent and induces rapid crystallization of uniform, ultra-smooth perovskite thin films. The mechanisms involved in the SSE process are studied further, and its versatility in depositing high quality thin films of controlled thicknesses (20 to 700 nm) and various compositions (CH3NH3PbI(3-x)Brx; x = 0, 1, 2, or 3) is demonstrated. Planar perovskite solar cells (PSCs) based on SSE-deposited CH3NH3PbI3 perovskite thin films deliver power conversion efficiency (PCE) up to 15.2%, and most notably an average PCE of 10.1% for PSCs with sub-100 nm semi-transparent perovskite thin films. The SSE method has generic appeal, and its key attributes-room-temperature process, rapid crystallization, large-area uniform deposition, film-thickness control, ultra-smoothness, and compositional versatility-make the SSE method potentially suitable for roll-to-roll scalable processing of hybrid-perovskite thin films for future multifunctional PSCs. C1 [Zhou, Yuanyuan; Wu, Wenwen; Vasiliev, Alexander L.; Padture, Nitin P.] Brown Univ, Sch Engn, Providence, RI 02912 USA. [Yang, Mengjin; Zhu, Kai] Natl Renewable Energy Lab, Chem & Mat Sci Ctr, Golden, CO 80401 USA. RP Padture, NP (reprint author), Brown Univ, Sch Engn, Providence, RI 02912 USA. EM kai.zhu@nrel.gov; nitin_padture@brown.edu RI Zhou, Yuanyuan/G-2173-2011; Vasiliev, Alexander/E-9855-2014; Padture, Nitin/A-9746-2009; OI Zhou, Yuanyuan/0000-0002-8364-4295; Vasiliev, Alexander/0000-0001-7884-4180; Padture, Nitin/0000-0001-6622-8559; Yang, Mengjin/0000-0003-2019-4298 FU National Science Foundation [DMR-1305913]; Brown University Graduate School; U.S. Department of Energy [DE-AC36-08-GO28308]; U.S. Department of Energy (DOE) SunShot Initiative under the Next Generation Photovoltaics 3 program [DE-FOA-0000990] FX This work was supported by a grant from the National Science Foundation (Grant no. DMR-1305913) and the Brown University Graduate School, and the work at the National Renewable Energy Laboratory was supported by the U.S. Department of Energy under Contract no. DE-AC36-08-GO28308. M.Y. and K.Z. acknowledge the support by the U.S. Department of Energy (DOE) SunShot Initiative under the Next Generation Photovoltaics 3 program (DE-FOA-0000990). We thank Dr H.F. Garces and Mr M. Strauss of Brown University, and Dr C.-S. Jiang of NREL, for experimental assistance. Disclosure: Y.Z. and N.P.P. have. led a provisional patent based on this work with the US Patent and Trademark Office. NR 31 TC 96 Z9 97 U1 37 U2 175 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7488 EI 2050-7496 J9 J MATER CHEM A JI J. Mater. Chem. A PY 2015 VL 3 IS 15 BP 8178 EP 8184 DI 10.1039/c5ta00477b PG 7 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA CF3IF UT WOS:000352441100063 ER PT J AU Jia, Y Sun, CH Peng, Y Fang, WQ Yan, XC Yang, DJ Zou, J Mao, SS Yao, XD AF Jia, Yi Sun, Chenghua Peng, Ye Fang, Wenqi Yan, Xuecheng Yang, Dongjiang Zou, Jin Mao, Samuel S. Yao, Xiangdong TI Metallic Ni nanocatalyst in situ formed from a metal-organic-framework by mechanochemical reaction for hydrogen storage in magnesium SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID PALLADIUM MEMBRANE; HYDRIDE; MGH2; DESTABILIZATION; SORPTION; DECOMPOSITION; NANOPARTICLES; DESORPTION; MECHANISM; SYSTEMS AB The facile and scalable fabrication of ultrafine (<5 nm) nanoparticles (NPs) as effective catalysts is the key for enhancing the kinetics of most hydrogen storage materials (HSMs). The direct fabrication of ultrafine NPs in HSMs is obviously a challenge because of the inevitable NPs agglomeration during the thermo-reduction. Herein, we report a mechanochemical-force-driven procedure for the one-step preparation of Ni NPs (2-3 nm) in a MgH2 matrix, which capitalizes on the in situ bottom-up reduction of Ni-MOF-74 in the presence of MgH2 as a reducing and sacrificing agent at room temperature. Both theoretical calculations and experimental investigations show that ultrafine Ni NPs are much more effective on catalytic hydrogenation/dehydrogenation in Mg due to the size effect. These findings may facilitate the fabrication of other catalyzed HSMs using different MOFs as catalyst precursors. C1 [Jia, Yi; Yao, Xiangdong] Univ Queensland, Sch Engn, ARC Ctr Excellence Funct Nanomat, St Lucia, Qld 4072, Australia. [Jia, Yi; Yao, Xiangdong] Univ Queensland, Australian Inst Bioengn & Nanotechnol, St Lucia, Qld 4072, Australia. [Jia, Yi; Zou, Jin] Univ Queensland, Sch Mech & Min Engn, St Lucia, Qld 4072, Australia. [Jia, Yi; Peng, Ye; Fang, Wenqi; Yan, Xuecheng; Yang, Dongjiang; Yao, Xiangdong] Griffith Univ, Queensland Micro & Nanotechnol Ctr QMNC, Nathan, Qld 4111, Australia. [Sun, Chenghua] Monash Univ, Fac Sci, Sch Chem, Clayton, Vic 3800, Australia. [Peng, Ye] Jilin Univ, State Key Lab Inorgan Synth & Preparat Chem, Changchun 130012, Peoples R China. [Mao, Samuel S.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Dept Mech Engn, Environm Energy Technol Div, Berkeley, CA 94720 USA. RP Yao, XD (reprint author), Univ Queensland, Sch Engn, ARC Ctr Excellence Funct Nanomat, St Lucia, Qld 4072, Australia. EM x.yao@griffith.edu.au RI Zou, Jin/B-3183-2009; Yao, Xiangdong/E-1259-2013; Griffith University, QMNC/I-5498-2013 OI Zou, Jin/0000-0001-9435-8043; FU Australia Research Council (ARC); Griffith University FX The financial support from Australia Research Council (ARC) is appreciated. Dr Yi Jia also thanks the Griffith University Post-doctoral and Research Fellowship and Griffith University New Research Grant. NR 37 TC 9 Z9 9 U1 11 U2 88 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7488 EI 2050-7496 J9 J MATER CHEM A JI J. Mater. Chem. A PY 2015 VL 3 IS 16 BP 8294 EP 8299 DI 10.1039/c5ta00278h PG 6 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA CF3ZZ UT WOS:000352489200011 ER PT J AU Soykal, II Wang, H Park, J Li, AP Liang, CD Schwartz, V AF Soykal, I. Ilgaz Wang, Hui Park, Jewook Li, An-Ping Liang, Chengdu Schwartz, Viviane TI Highly dispersed buckybowls as model carbocatalysts for C-H bond activation SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID OXIDATIVE DEHYDROGENATION REACTIONS; CARBON CATALYSTS; HETEROGENEOUS CATALYSIS; THERMAL-STABILITY; N-BUTANE; FULLERENE; ETHYLBENZENE; C-60; ISOBUTANE; RAMAN AB Fullerene-derived buckybowl fractions dispersed on mesoporous silica constitute an ideal model for studying the catalysis of graphitic forms of carbon since the dispersed carbon nanostructures contain a high ratio of edge defects and curvature induced by non-six-membered rings. Dispersion of the active centers on an easily accessible high surface area material allowed for high density of surface active sites associated with oxygenated structures. This report illustrates a facile method of creating model polycyclic aromatic nano-structures that are not only active for alkane C-H bond activation and oxidative dehydrogenation but also can be practical catalysts to be eventually used in industry. C1 [Soykal, I. Ilgaz; Wang, Hui; Park, Jewook; Li, An-Ping; Liang, Chengdu; Schwartz, Viviane] 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, Oak Ridge, TN 37831 USA. EM liangcn@ornl.gov; schwartzv@ornl.gov RI Park, Jewook/N-2856-2015; Li, An-Ping/B-3191-2012 OI Li, An-Ping/0000-0003-4400-7493 FU Center for Nanophase Materials Sciences, at Oak Ridge National Laboratory by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy FX This research was supported by 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 39 TC 0 Z9 0 U1 4 U2 22 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7488 EI 2050-7496 J9 J MATER CHEM A JI J. Mater. Chem. A PY 2015 VL 3 IS 16 BP 8667 EP 8675 DI 10.1039/c5ta00898k PG 9 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA CF3ZZ UT WOS:000352489200032 ER PT J AU Engmann, S Bokel, FA Herzing, AA Ro, HW Girotto, C Caputo, B Hoven, CV Schaible, E Hexemer, A DeLongchamp, DM Richter, LJ AF Engmann, Sebastian Bokel, Felicia A. Herzing, Andrew A. Ro, Hyun Wook Girotto, Claudio Caputo, Bruno Hoven, Corey V. Schaible, Eric Hexemer, Alexander DeLongchamp, Dean M. Richter, Lee J. TI Real-time X-ray scattering studies of film evolution in high performing small-molecule-fullerene organic solar cells SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID MORPHOLOGY CONTROL; BLEND FILMS; EFFICIENCY; ADDITIVES; DESIGN AB We have studied the influence of the formulation additive 1,8-diiodooctane (DIO) on the structural evolution of bulk heterojunction (BHJ) films based the small molecule donor 7,7'-(4,4-bis(2-ethylhexyl)-4H-silolo[3,2-b:4,5-b']dithiophene-2,6-diyl)bis(6-fluoro-5-(5'-hexyl-[2,2'-bithiophen]-5-yl)benzo[c][1,2,5]thiadiazole) (p-DTS(FBTTh2)(2)) and phenyl-C-71-butyric-acid-methyl ester ([70]PCBM). Real-time, in situ, grazing-incidence X-ray scattering experiments allow us to characterize the development of crystalline order via diffraction and phase separation via small angle scattering. The performance of p-DTS(FBTTh2)(2) based solar cells exhibits a distinct optimum with respect to volume fraction of DIO in the coating solution, unlike many polymer-fullerene systems that exhibit plateaus in performance above a certain additive volume fraction. Increasing the DIO volume fraction increases the crystallinity of p-DTS(FBTTh2)(2) and dramatically increases the phase separation length scale even at small DIO amounts. These results suggest that the existence of an optimal DIO amount is a consequence of the phase separation length scale and its relationship to the optimal length for exciton dissociation. The effects of DIO on the time evolution of the drying films indicates that it acts as both a solvent and a plasticizer for p-DTS(FBTTh2)(2), controlling its nucleation density and promoting its crystal growth. C1 [Engmann, Sebastian; Bokel, Felicia A.; Herzing, Andrew A.; Ro, Hyun Wook; DeLongchamp, Dean M.; Richter, Lee J.] NIST, Mat Sci Engn Div, Gaithersburg, MD 20899 USA. [Girotto, Claudio; Caputo, Bruno; Hoven, Corey V.] NEXT Energy Technol Inc, Santa Barbara, CA USA. [Schaible, Eric; Hexemer, Alexander] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. RP DeLongchamp, DM (reprint author), NIST, Mat Sci Engn Div, Gaithersburg, MD 20899 USA. EM dean.delongchamp@nist.gov; lee.richter@nist.gov RI Richter, Lee/N-7730-2016 OI Richter, Lee/0000-0002-9433-3724 FU ARRA; NIST/National Research Council (NRC); Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231] FX Materials preparation and ellipsometric studies were performed in the NIST Organic Photovoltaic Integrated Measurement Facility funded through ARRA. FB acknowledges support of a NIST/National Research Council (NRC) postdoctoral fellowship. Beamline 7.3.3 of the Advanced Light Source is supported by the Director of the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under contract no. DE-AC02-05CH11231. NR 34 TC 16 Z9 16 U1 6 U2 30 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7488 EI 2050-7496 J9 J MATER CHEM A JI J. Mater. Chem. A PY 2015 VL 3 IS 16 BP 8764 EP 8771 DI 10.1039/c5ta00935a PG 8 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA CF3ZZ UT WOS:000352489200044 ER PT J AU Dudson, BD Allen, A Breyiannis, G Brugger, E Buchanan, J Easy, L Farley, S Joseph, I Kim, M McGann, AD Omotani, JT Umansky, MV Walkden, NR Xia, T Xu, XQ AF Dudson, B. D. Allen, A. Breyiannis, G. Brugger, E. Buchanan, J. Easy, L. Farley, S. Joseph, I. Kim, M. McGann, A. D. Omotani, J. T. Umansky, M. V. Walkden, N. R. Xia, T. Xu, X. Q. TI BOUT plus plus : Recent and current developments SO JOURNAL OF PLASMA PHYSICS LA English DT Article ID BOUNDARY PLASMAS; SIMULATIONS; TURBULENCE; TOKAMAK; TRANSPORT; SOL; RECONSTRUCTION; PHYSICS AB BOUT++ is a 3D nonlinear finite-difference plasma simulation code, capable of solving quite general systems of Partial Differential Equations (PDEs), but targeted particularly on studies of the edge region of tokamak plasmas. BOUT++ is publicly available, and has been adopted by a growing number of researchers worldwide. Here we present improvements which have been made to the code since its original release, both in terms of structure and its capabilities. Some recent applications of these methods are reviewed, and areas of active development are discussed. We also present algorithms and tools which have been developed to enable creation of inputs from analytic expressions and experimental data, and for processing and visualisation of output results. This includes a new tool HYPNOTOAD for the creation of meshes from experimental equilibria. Algorithms have been implemented in BOUT++ to solve a range of linear algebraic problems encountered in the simulation of reduced Magnetohydrodynamics (MHD) and gyro-fluid models: A preconditioning scheme is presented which enables the plasma potential to be calculated efficiently using iterative methods supplied by the PETSc library (the Portable, Extensible Toolkit for Scientific Computation) (Balay et al. 2014), without invoking the Boussinesq approximation. Scaling studies are also performed of a linear solver used as part of physics-based preconditioning to accelerate the convergence of implicit time-integration schemes. C1 [Dudson, B. D.; Allen, A.; Easy, L.; McGann, A. D.; Walkden, N. R.] Univ York, York Plasma Inst, Dept Phys, York YO10 5DD, N Yorkshire, England. [Breyiannis, G.] Japan Atom Energy Agcy, Rokkasho Fus Inst, Rokkasho 0393212, Japan. [Brugger, E.; Joseph, I.; Umansky, M. V.; Xia, T.] Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. [Buchanan, J.; Easy, L.; Omotani, J. T.; Walkden, N. R.] Culham Sci Ctr, CCFE, Abingdon OX14 3DB, Oxon, England. [Farley, S.] IIT, Dept Math, Chicago, IL 60616 USA. [Kim, M.] POSTECH, Dept Phys, Pohang 790784, Gyeongbuk, South Korea. [Xia, T.] Chinese Acad Sci, Inst Plasma Phys, Hefei, Peoples R China. RP Dudson, BD (reprint author), Univ York, York Plasma Inst, Dept Phys, York YO10 5DD, N Yorkshire, England. EM benjamin.dudson@york.ac.uk OI Dudson, Benjamin/0000-0002-0094-4867 FU EPSRC [EP/K006940/1, EP/L000237/1]; EURATOM Mobility FX This work was funded by EPSRC grant EP/K006940/1 using HECToR computing resources through the Plasma HEC consortium grant EP/L000237/1. EURATOM Mobility support is gratefully acknowledged. The views and opinions expressed herein do not necessarily reflect those of the European Commission. NR 66 TC 6 Z9 6 U1 4 U2 18 PU CAMBRIDGE UNIV PRESS PI NEW YORK PA 32 AVENUE OF THE AMERICAS, NEW YORK, NY 10013-2473 USA SN 0022-3778 EI 1469-7807 J9 J PLASMA PHYS JI J. Plasma Phys. PD JAN PY 2015 VL 81 AR 365810104 DI 10.1017/S0022377814000816 PN 1 PG 24 WC Physics, Fluids & Plasmas SC Physics GA CE9WF UT WOS:000352193400025 ER PT J AU Gilmore, M Lynn, AG Desjardins, TR Zhang, Y Watts, C Hsu, SC Betts, S Kelly, R Schamiloglu, E AF Gilmore, M. Lynn, A. G. Desjardins, T. R. Zhang, Y. Watts, C. Hsu, S. C. Betts, S. Kelly, R. Schamiloglu, E. TI The HelCat basic plasma science device SO JOURNAL OF PLASMA PHYSICS LA English DT Article ID POTENTIAL RELAXATION INSTABILITY; SPHEROMAK INJECTION; DISCHARGE PLASMA; EXCITATION; TRANSPORT; TOKAMAK; LAYER; SHEAR; UCLA AB The Helicon-Cathode(HelCat) device is a medium-size linear experiment suitable for a wide range of basic plasma science experiments in areas such as electrostatic turbulence and transport, magnetic relaxation, and high power microwave (HPM)plasma interactions. The HelCat device is based on dual plasma sources located at opposite ends of the 4 m long vacuum chamber - an RF helicon source at one end and a thermionic cathode at the other. Thirteen coils provide an axial magnetic field B <= 0.220 T that can be configured individually to give various magnetic configurations (e.g. solenoid, mirror, cusp). Additional plasma sources, such as a compact coaxial plasma gun, are also utilized in some experiments, and can be located either along the chamber for perpendicular (to the background magnetic field) plasma injection, or at one of the ends for parallel injection. Using the multiple plasma sources, a wide range of plasma parameters can be obtained. Here, the HelCat device is described in detail and some examples of results from previous and ongoing experiments are given. Additionally, examples of planned experiments and device modifications are also discussed. C1 [Gilmore, M.; Lynn, A. G.; Desjardins, T. R.; Zhang, Y.; Watts, C.; Betts, S.; Kelly, R.; Schamiloglu, E.] Univ New Mexico, Dept Elect & Comp Engn, Albuquerque, NM 87131 USA. [Watts, C.] ITER Org, St Paul Les Durance, France. [Hsu, S. C.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Gilmore, M (reprint author), Univ New Mexico, Dept Elect & Comp Engn, Albuquerque, NM 87131 USA. EM mgilmore@unm.edu OI Hsu, Scott/0000-0002-6737-4934 FU US National Science Foundation; US Department of Energy Office of Science; University of New Mexico FX The authors would like to acknowledge Paolo Ricci for supplying the LSS code and for many useful discussions and Tyler Wynkoop for assistance with figures. We also thank Glen Wurden of Los Alamos National Laboratory for the loan of the Hadland camera used for Figs 16 and 17. The RF-Langmuir turbulence experiment was suggested by Evgeny Mishen. This work was supported by the US National Science Foundation, the US Department of Energy Office of Science, and the University of New Mexico. NR 48 TC 2 Z9 2 U1 2 U2 9 PU CAMBRIDGE UNIV PRESS PI NEW YORK PA 32 AVENUE OF THE AMERICAS, NEW YORK, NY 10013-2473 USA SN 0022-3778 EI 1469-7807 J9 J PLASMA PHYS JI J. Plasma Phys. PD JAN PY 2015 VL 81 AR 345810104 DI 10.1017/S0022377814000919 PN 1 PG 23 WC Physics, Fluids & Plasmas SC Physics GA CE9WF UT WOS:000352193400021 ER PT J AU Le, A Egedal, J Daughton, W Roytershteyn, V Karimabadi, H Forest, C AF Le, A. Egedal, J. Daughton, W. Roytershteyn, V. Karimabadi, H. Forest, C. TI Transition in electron physics of magnetic reconnection in weakly collisional plasma SO JOURNAL OF PLASMA PHYSICS LA English DT Article ID ACCELERATION; TRANSPORT; FIELDS AB Using particle-in-cell (PIC) simulations with a Monte Carlo treatment of the Coulomb collision operator, we study the transition in electron dynamics of magnetic reconnection for various levels of collisionality. The weakly collisional cases considered all fall into the so-called Hall or kinetic regime. Nevertheless, collisions may still alter the electron kinetic physics characteristic of collisionless reconnection, where adiabatic trapping energizes the electrons and leads to strong anisotropy of the electron velocity distribution and pressure. This anisotropy can support extended current sheets, associated with secondary island formation and turbulent flux rope interactions in three dimensional systems. The collisional simulations demonstrate how weak collisions may modify or eliminate these electron structures in the kinetic regimes. While the reconnection rate is not sensitive to the collisionality in the range studied, we find that increasing collisionality reduces the level of electron energization near the reconnection site. Finally, the results provide guidance for new laboratory reconnection experiments that will access the weakly collisional regimes. C1 [Le, A.; Roytershteyn, V.; Karimabadi, H.] SciberQuest Inc, Del Mar, CA 92014 USA. [Le, A.] Space Sci Inst, Ctr Space Plasma Phys, Boulder, CO 80301 USA. [Egedal, J.; Forest, C.] Univ Wisconsin, Dept Phys, Madison, WI 53706 USA. [Daughton, W.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Le, A (reprint author), SciberQuest Inc, Del Mar, CA 92014 USA. EM ale@spacescience.org RI Daughton, William/L-9661-2013; OI Roytershteyn, Vadim/0000-0003-1745-7587 FU NASA [NNH11CC65C, NNX14AL38G, NNX10AL11G]; NSF [1202152, ATM0802380, OCI0904734] FX A.L., H.K., and V.R.'s work was supported by NASA grants NNH11CC65C and NNX14AL38G and NSF award 1202152. J.E. acknowledges support through NASA grant NNX10AL11G and NSF Grants ATM0802380 and OCI0904734. W.D.'s work was supported by the NASA Heliophysics Theory Program. Simulations were performed on Kraken provided by NSF at NICS and on Pleiades provided by NASA's HEC program, and using resources from the Los Alamos Institutional Computing program. NR 33 TC 4 Z9 4 U1 0 U2 3 PU CAMBRIDGE UNIV PRESS PI NEW YORK PA 32 AVENUE OF THE AMERICAS, NEW YORK, NY 10013-2473 USA SN 0022-3778 EI 1469-7807 J9 J PLASMA PHYS JI J. Plasma Phys. PD JAN PY 2015 VL 81 AR 305810108 DI 10.1017/S0022377814000907 PN 1 PG 16 WC Physics, Fluids & Plasmas SC Physics GA CE9WF UT WOS:000352193400008 ER PT J AU Palmer, CAJ Dover, NP Pogorelsky, I Streeter, MJV Najmudin, Z AF Palmer, Charlotte A. J. Dover, Nicholas P. Pogorelsky, Igor Streeter, Matthew J. V. Najmudin, Zulfikar TI Manipulation of laser-generated energetic proton spectra in near critical density plasma SO JOURNAL OF PLASMA PHYSICS LA English DT Article ID ION-ACCELERATION; BEAMS; TARGETS; ABSORPTION; ELECTRON; PULSES AB We present simulations that demonstrate the production of quasi-monoenergetic proton bunches from the interaction of a CO2 laser pulse train with a near-critical density hydrogen plasma. The multi-pulse structure of the laser leads to a steepening of the plasma density gradient, which the simulations show is necessary for the formation of narrow-energy spread proton bunches. Laser interactions with a long, front surface, scale-length (>> c/omega(p)) plasma, with linear density gradient, were observed to generate proton beams with a higher maximum energy, but a much broader spectrum compared to step-like density profiles. In the step-like cases, a peak in the proton energy spectra was formed and seen to scale linearly with the ratio of laser intensity to plasma density. C1 [Palmer, Charlotte A. J.; Streeter, Matthew J. V.] Deutsch Elektronen Synchrotron DESY, D-22607 Hamburg, Germany. [Palmer, Charlotte A. J.; Dover, Nicholas P.; Najmudin, Zulfikar] Univ London Imperial Coll Sci Technol & Med, Blackett Lab, John Adams Inst Accelerator Sci, London SW7 2AZ, England. [Pogorelsky, Igor] Brookhaven Natl Lab, Accelerator Test Facil, Upton, NY 11973 USA. RP Palmer, CAJ (reprint author), Deutsch Elektronen Synchrotron DESY, D-22607 Hamburg, Germany. EM charlotte.palmer@desy.de OI Dover, Nicholas/0000-0003-0420-3940 FU EPSRC [EP/E035728/1, EP/K022415/1]; STFC [ST/J002062/1]; DOE [DE-FG0207ER41488] FX The authors would like to acknowledge the assistance of the ATF staff and experimental collaborators in the performance of the experiment and the OSIRIS collaboration for access to the simulation code. Computing services were provided by Imperial College HPC. The work was funded by EPSRC grants EP/E035728/1, EP/K022415/1, STFC grant ST/J002062/1 and DOE grant DE-FG0207ER41488. NR 29 TC 0 Z9 0 U1 0 U2 11 PU CAMBRIDGE UNIV PRESS PI NEW YORK PA 32 AVENUE OF THE AMERICAS, NEW YORK, NY 10013-2473 USA SN 0022-3778 EI 1469-7807 J9 J PLASMA PHYS JI J. Plasma Phys. PD JAN PY 2015 VL 81 AR 365810103 DI 10.1017/S0022377814000798 PN 1 PG 9 WC Physics, Fluids & Plasmas SC Physics GA CE9WF UT WOS:000352193400024 ER PT J AU Scime, EE Keiter, PA Balkey, MM Kline, JL Sun, X Keesee, AM Hardin, RA Biloiu, IA Houshmandyar, S Thakur, SC Carr, J Galante, M McCarren, D Sears, S AF Scime, E. E. Keiter, P. A. Balkey, M. M. Kline, J. L. Sun, X. Keesee, A. M. Hardin, R. A. Biloiu, I. A. Houshmandyar, S. Thakur, S. Chakraborty Carr, J., Jr. Galante, M. McCarren, D. Sears, S. TI The hot hELicon eXperiment (HELIX) and the large experiment on instabilities and anisotropy (LEIA) SO JOURNAL OF PLASMA PHYSICS LA English DT Article ID ION TEMPERATURE ANISOTROPY; PLASMA; MAGNETOSHEATH; FREQUENCY; ELECTRON; DEVICE AB The West Virginia University Hot hELIcon eXperiment (HELIX) provides variable density and ion temperature plasmas, with controllable levels of thermal anisotropy, for space relevant laboratory experiments in the Large Experiment on Instabilities and Anisotropy (LEIA) as well as fundamental studies of helicon source physics in HELIX. Through auxiliary ion heating, the ion temperature anisotropy (T-perpendicular to/T-parallel to) is variable from 1 to 20 for parallel plasma beta (beta = 8 pi nkT(i parallel to)/B-2) values that span the range of 0.0001 to 0.01 in LEIA. The ion velocity distribution function is measured throughout the discharge volume in steady-state and pulsed plasmas with laser induced fluorescence (LIF). The wavelengths of very short wavelength electrostatic fluctuations are measured with a coherent microwave scattering system. Operating at low neutral pressures triggers spontaneous formation of a current-free electric double layer. Ion acceleration through the double layer is detected through LIF. LIF-based velocity space tomography of the accelerated beam provides a two-dimensional mapping of the bulk and beam ion distribution functions. The driving frequency for the m = 1 helical antenna is continuously variable from 8.5 to 16 MHz and frequency dependent variations of the RF coupling to the plasma allow the spontaneously appearing double layers to be turned on and off without modifying the plasma collisionality or magnetic field geometry. Single and multi-species plasmas are created with argon, helium, nitrogen, krypton, and xenon. The noble gas plasmas have steep neutral density gradients, with ionization levels reaching 100% in the core of the plasma source. The large plasma density in the source enables the study of Aflven waves in the HELIX device. C1 [Scime, E. E.; Balkey, M. M.; Keesee, A. M.; McCarren, D.; Sears, S.] Univ Virginia, Dept Phys & Astron, Morgantown, WV 26506 USA. [Keiter, P. A.] Univ Michigan, Dept Atmospher & Space Sci, Ann Arbor, MI 48109 USA. [Kline, J. L.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Sun, X.] Univ Sci & Technol China, Dept Modern Phys, Hefei 230026, Anhui, Peoples R China. [Hardin, R. A.] Wacker Polysilicon North Amer LLC, Charleston, TN 37310 USA. [Biloiu, I. A.] US Army Res Lab, Adelphi, MD 20783 USA. [Houshmandyar, S.] Gonzaga Univ, Dept Phys, Spokane, WA 99258 USA. [Thakur, S. Chakraborty] Univ Calif San Diego, Energy Res Ctr, San Diego, CA 92093 USA. [Carr, J., Jr.] Texas Lutheran Univ, Dept Phys, Seguin, TX 78155 USA. [Galante, M.] Univ Wisconsin, Dept Phys, Madison, WI 53706 USA. RP Scime, EE (reprint author), Univ Virginia, Dept Phys & Astron, Morgantown, WV 26506 USA. EM escime@wvu.edu OI Keesee, Amy/0000-0002-9719-3229; Kline, John/0000-0002-2271-9919 FU NSF [PHY-0611571] FX This work was supported by NSF award PHY-0611571. The authors thank one referee for suggesting the additional comparison with the theory of Reference 51 that is now shown in Fig. 15. NR 45 TC 4 Z9 4 U1 0 U2 11 PU CAMBRIDGE UNIV PRESS PI NEW YORK PA 32 AVENUE OF THE AMERICAS, NEW YORK, NY 10013-2473 USA SN 0022-3778 EI 1469-7807 J9 J PLASMA PHYS JI J. Plasma Phys. PD JAN PY 2015 VL 81 AR 345810103 DI 10.1017/S0022377814000890 PN 1 PG 22 WC Physics, Fluids & Plasmas SC Physics GA CE9WF UT WOS:000352193400020 ER PT J AU Willingale, L Nagel, SR Thomas, AGR Bellei, C Clarke, RJ Dangor, AE Heathcote, R Kaluza, MC Kamperidis, C Kneip, S Krushelnick, K Lopes, N Mangles, SPD Nazarov, W Nilson, PM Najmudin, Z AF Willingale, L. Nagel, S. R. Thomas, A. G. R. Bellei, C. Clarke, R. J. Dangor, A. E. Heathcote, R. Kaluza, M. C. Kamperidis, C. Kneip, S. Krushelnick, K. Lopes, N. Mangles, S. P. D. Nazarov, W. Nilson, P. M. Najmudin, Z. TI Characterization of laser-driven proton beams from near-critical density targets using copper activation SO JOURNAL OF PLASMA PHYSICS LA English DT Article ID PLASMA INTERACTIONS; SOLID INTERACTIONS; GENERATION; PULSES; ION AB Copper activation was used to characterize high-energy proton beam acceleration from near-critical density plasma targets. An enhancement was observed when decreasing the target density, which is indicative for an increased laser-accelerated hot electron density at the rear target-vacuum boundary. This is due to channel formation and collimation of the hot electrons inside the target. Particle-in-cell simulations support the experimental observations and show the correlation between channel depth and longitudinal electric field strength is directly correlated with the proton acceleration. C1 [Willingale, L.; Thomas, A. G. R.; Krushelnick, K.] Univ Michigan, Ctr Ultrafast Opt Sci, Ann Arbor, MI 48109 USA. [Nagel, S. R.; Bellei, C.] Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. [Clarke, R. J.; Heathcote, R.] Rutherford Appleton Lab, Cent Laser Facil, Chilton OX11 0QX, Oxon, England. [Dangor, A. E.; Kamperidis, C.; Kneip, S.; Lopes, N.; Mangles, S. P. D.; Najmudin, Z.] Univ London Imperial Coll Sci Technol & Med, Blackett Lab, John Adams Inst Accelerator Sci, London SW7 2AZ, England. [Kaluza, M. C.] Inst Opt & Quantenelekt, D-07743 Jena, Germany. [Kaluza, M. C.] Helmholtz Inst Jena, D-07743 Jena, Germany. [Lopes, N.] Inst Super Tecn, GoLP, Lisbon, Portugal. [Nazarov, W.] Univ St Andrews, High Energy Laser Mat R&D Lab, St Andrews KY16 9ST, Fife, Scotland. [Nilson, P. M.] Univ Rochester, Laser Energet Lab, Rochester, NY 14623 USA. RP Willingale, L (reprint author), Univ Michigan, Ctr Ultrafast Opt Sci, 2200 Bonisteel Blvd, Ann Arbor, MI 48109 USA. EM wlouise@umich.edu RI Mangles, Stuart/F-9070-2014; Lopes, Nelson/C-6540-2009; OI Mangles, Stuart/0000-0003-2443-4201; Lopes, Nelson/0000-0001-8355-4727; Thomas, Alexander/0000-0003-3206-8512 FU EPSRC [GR/T25934/01] FX The authors gratefully acknowledge the staff of the Central Laser Facility (RAL) for technical assistance and the Osiris consortium (UCLA and IST) for the use of the code. The work was funded by EPSRC grant GR/T25934/01. NR 26 TC 1 Z9 1 U1 3 U2 18 PU CAMBRIDGE UNIV PRESS PI NEW YORK PA 32 AVENUE OF THE AMERICAS, NEW YORK, NY 10013-2473 USA SN 0022-3778 EI 1469-7807 J9 J PLASMA PHYS JI J. Plasma Phys. PD JAN PY 2015 VL 81 AR 365810102 DI 10.1017/S002237781400066X PN 1 PG 12 WC Physics, Fluids & Plasmas SC Physics GA CE9WF UT WOS:000352193400023 ER PT J AU Chamorro, LP Hong, J Gangodagamage, C AF Chamorro, L. P. Hong, J. Gangodagamage, C. TI On the scale-to-scale coupling between a full-scale wind turbine and turbulence SO JOURNAL OF TURBULENCE LA English DT Article DE field experiment; flow-structure interaction; turbine loading; wavelet analysis; wind turbine ID MULTIFRACTAL FORMALISM; DEVELOPED TURBULENCE; SIGNALS; ORGANIZATION; WAVELETS; VELOCITY; LOADS; SHEAR; LAYER AB The scale-dependent response of an instrumented full-scale wind turbine is studied under neutrally stratified conditions. The analysis is focused on the linkage between the incoming flow, turbine power output and foundation strain. Wind speed, measured from sonic anemometers installed on a meteorological tower, and foundation strain were sampled at 20 Hz, while the turbine power was sampled at 1 Hz. A wavelet framework and structure function are used to obtain cross correlations among flow turbulence, turbine power and strain across scales as well as to quantify intermittent signatures in both flow and turbine quantities. Results indicate that correlation between the streamwise velocity component of the wind flow and turbine power is maximised across all scales larger than the rotor radius for wind measured at the turbine hub height. The characteristic time lag associated with maximum correlation is shown to be consistent with the Taylor's hypothesis for turbulent scales smaller than the separation between the meteorological tower and the turbine. However, it decreases with increasing scale size and diminishes to zero at scales on the order of the boundary layer thickness. Turbine power and strain fluctuations exhibited practically the same behaviour at scales larger than two rotor diameters. At those scales, the cross correlation between these quantities resulted similar to 0.99 and remains still over 0.9 at the scale of rotor radius. Below this scale, the correlation decreases logarithmically with scale. The strong linkage between power and strain for all the relevant scales would eventually allow the analysis of dynamic forcing on the foundation based on the power output. Intermittency on the flow is shown to be transferred and amplified by the turbine, leading to highly intermittent power output. C1 [Chamorro, L. P.] Univ Illinois, Dept Mech Sci & Engn, Urbana, IL 61801 USA. [Hong, J.] Univ Minnesota, Dept Mech Engn, St Anthony Falls Lab, Minneapolis, MN 55455 USA. [Gangodagamage, C.] Univ Calif Davis, Dept Land Air & Water Resources, Davis, CA 95616 USA. [Gangodagamage, C.] Los Alamos Natl Lab, Los Alamos, NM USA. RP Chamorro, LP (reprint author), Univ Illinois, Dept Mech Sci & Engn, Urbana, IL 61801 USA. EM lpchamo@illinois.edu FU US Department of Energy DOE [DE-EE0002980] FX This work was financially supported by the US Department of Energy DOE [DE-EE0002980]. NR 46 TC 1 Z9 1 U1 2 U2 8 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 2015 VL 16 IS 7 BP 617 EP 632 DI 10.1080/14685248.2015.1021472 PG 16 WC Mechanics; Physics, Fluids & Plasmas SC Mechanics; Physics GA CF5PW UT WOS:000352610300002 ER PT J AU Smith, BE Roder, PB Zhou, XZ Pauzauskie, PJ AF Smith, Bennett E. Roder, Paden B. Zhou, Xuezhe Pauzauskie, Peter J. TI Nanoscale materials for hyperthermal theranostics SO NANOSCALE LA English DT Article ID PHOTOTHERMAL CANCER-THERAPY; WALLED CARBON NANOTUBES; MAGNETIC FLUID HYPERTHERMIA; UP-CONVERSION NANOPARTICLES; SURFACE-PLASMON RESONANCE; CORE-SHELL NANOCOMPOSITES; IRON-OXIDE NANOPARTICLES; 980 NM-LASER; IN-VIVO; DRUG-DELIVERY AB Recently, the use of nanoscale materials has attracted considerable attention with the aim of designing personalized therapeutic approaches that can enhance both spatial and temporal control over drug release, permeability, and uptake. Potential benefits to patients include the reduction of overall drug dosages, enabling the parallel delivery of different pharmaceuticals, and the possibility of enabling additional functionalities such as hyperthermia or deep-tissue imaging (LIF, PET, etc.) that complement and extend the efficacy of traditional chemotherapy and surgery. This mini-review is focused on an emerging class of nanometer-scale materials that can be used both to heat malignant tissue to reduce angiogenesis and DNA-repair while simultaneously offering complementary imaging capabilities based on radioemission, optical fluorescence, magnetic resonance, and photoacoustic methods. C1 [Smith, Bennett E.] Univ Washington, Dept Chem, Seattle, WA 98195 USA. [Roder, Paden B.; Zhou, Xuezhe; Pauzauskie, Peter J.] Univ Washington, Dept Mat Sci & Engn, Seattle, WA 98195 USA. [Pauzauskie, Peter J.] Pacific NW Natl Lab, Fundamental & Computat Sci Directorate, Richland, WA 99352 USA. RP Pauzauskie, PJ (reprint author), Univ Washington, Dept Mat Sci & Engn, Seattle, WA 98195 USA. EM peterpz@u.washington.edu FU Air Force Office of Scientific Research [FA95501210400]; University of Washington; NIH/NCI [T32CA138312]; NSF [DGE-1256082]; Pacific Northwest National Laboratory; US DOE [DE-AC 06-76RLO 1830] FX This research was made possible by a grant from the Air Force Office of Scientific Research Young Investigator Program (contract #FA95501210400) and start-up funding from the University of Washington. B. E. S. acknowledges support from an NIH/NCI T32 training grant (T32CA138312). P. B. R. thanks the NSF for a Graduate Research Fellowship under grant number DGE-1256082. P. J. P. gratefully acknowledges support from the Pacific Northwest National Laboratory which is operated by the Battelle Memorial Institute for the US DOE under contract DE-AC 06-76RLO 1830. NR 181 TC 11 Z9 11 U1 9 U2 62 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2040-3364 EI 2040-3372 J9 NANOSCALE JI Nanoscale PY 2015 VL 7 IS 16 BP 7115 EP 7126 DI 10.1039/c4nr06164k PG 12 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA CF9SC UT WOS:000352905700022 PM 25816102 ER PT J AU Li, RZ Hu, AM Bridges, D Zhang, T Oakes, KD Peng, R Tumuluri, U Wu, ZL Feng, ZL AF Li, Ruo-Zhou Hu, Anming Bridges, Denzel Zhang, Tong Oakes, Ken D. Peng, Rui Tumuluri, Uma Wu, Zili Feng, Zhili TI Robust Ag nanoplate ink for flexible electronics packaging SO NANOSCALE LA English DT Article ID CONDUCTIVE ADHESIVES; ROOM-TEMPERATURE; LARGE-SCALE; SILVER; NANOPARTICLES; NANOWIRES; COMPOSITES; NANOPRISMS; PAPER; PASTE AB Nanoinks are currently a topic of heightened interest with respect to low temperature bonding processes and printable electronics. We have developed an innovative polyvinylpyrrolidone (PVP)-stabilized Ag nanoplate ink amenable to very strong low temperature packaging, and investigated the relationship between bonding strength and electrical conductivity post-bonding. PVP shell plastic deformations observed in failure microcracks with the formation of PVP nanofibers, revealed bonding strength at low temperatures (<250 degrees C) was primarily due to adhesive bonding. It is found that, utilizing photonic sintering, similar to 70 degrees C reduction of transformation temperature from adhesive to metallic bonding was achieved compared to that of thermal sintering. A numerical simulation was developed to better understand the influences of the light-induced heat generation, which demonstrated near-infrared light can facilitate sintering. Bonding strengths of 27 MPa were achieved at room temperatures, and 29.4 MPa at 210 degrees C with photonic sintering. Moreover, the anisotropic resistivity was observed with different thermal dependences. These results demonstrate Ag nanoplate inks have potential for low temperature 3D interconnections in lead-free microcircuits, flexible electronic packaging, and diverse sensing applications. C1 [Li, Ruo-Zhou; Zhang, Tong] Southeast Univ, Sch Elect Sci & Engn, Key Lab Microinertial Instrument & Adv Nav Techno, Minist Educ, Nanjing 210096, Jiangsu, Peoples R China. [Li, Ruo-Zhou; Hu, Anming; Bridges, Denzel] Univ Tennessee, Dept Mech Aerosp & Biomed Engn, Knoxville, TN 37996 USA. [Li, Ruo-Zhou; Zhang, Tong] Southeast Univ, Suzhou Res Inst, Suzhou Key Lab Met Nanooptoelect Technol, Suzhou 215123, Peoples R China. [Oakes, Ken D.] Cape Breton Univ, Dept Biol, Verschuren Ctr, Sydney, NSW B1P 6L2, Australia. [Peng, Rui; Tumuluri, Uma; Wu, Zili] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. [Peng, Rui; Tumuluri, Uma; Wu, Zili] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. [Feng, Zhili] Oak Ridge Natl Lab, Mat Sci & Technol Div, Mat Proc & Joining, Oak Ridge, TN 37831 USA. RP Hu, AM (reprint author), Univ Tennessee, Dept Mech Aerosp & Biomed Engn, Knoxville, TN 37996 USA. EM ahu3@utk.edu; tzhang@seu.edu.cn RI Hu, Anming/E-7370-2011; Wu, Zili/F-5905-2012; Feng, Zhili/H-9382-2012; Peng, Rui/J-3781-2016 OI Hu, Anming/0000-0001-9794-0549; Wu, Zili/0000-0002-4468-3240; Feng, Zhili/0000-0001-6573-7933; Peng, Rui/0000-0002-1686-9574 FU University of Tennessee; NSFC [61307066]; Doctoral Fund of Ministry of Education of China [20110092110016, 20130092120024]; Natural Science Foundation of Jiangsu Province [BK20130630]; National Basic Research Program of China (973 Program) [2011CB302004]; Foundation of Key Laboratory of Micro-Inertial Instrument and Advanced Navigation Technology, Ministry of Education, China [201204]; Education Commission [KZ40005001] FX We appreciate the research initiative funding provided by the University of Tennessee as a new hire package to AH. Part of the work including the thermal analysis and FTIR was conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility. This work is also in part supported by NSFC under grant number 61307066, Doctoral Fund of Ministry of Education of China under grant number 20110092110016 and 20130092120024, Natural Science Foundation of Jiangsu Province under grant number BK20130630, the National Basic Research Program of China (973 Program) under grant number 2011CB302004 and the Foundation of Key Laboratory of Micro-Inertial Instrument and Advanced Navigation Technology, Ministry of Education, China under grant number 201204, a strategic research project (KZ40005001) of the Education Commission. We also appreciate Dr John R Dunlap for the assistance in FIB sample preparation and TEM (JIAM Analytical Instrument Facilities, University of Tennessee at Knoxville). NR 42 TC 18 Z9 18 U1 16 U2 98 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2040-3364 EI 2040-3372 J9 NANOSCALE JI Nanoscale PY 2015 VL 7 IS 16 BP 7368 EP 7377 DI 10.1039/c5nr00312a PG 10 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA CF9SC UT WOS:000352905700055 PM 25824693 ER PT J AU Ulvestad, A Clark, JN Singer, A Vine, D Cho, HM Harder, R Meng, YS Shpyrko, OG AF Ulvestad, Andrew Clark, Jesse N. Singer, Andrej Vine, David Cho, H. M. Harder, Ross Meng, Ying Shirley Shpyrko, Oleg G. TI In situ strain evolution during a disconnection event in a battery nanoparticle SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID LITHIUM-ION BATTERIES; LIFEPO4 NANOPARTICLES; CATHODE MATERIALS; COHERENCY STRAIN; PHASE-SEPARATION; ELECTROLYTE; DYNAMICS; ENERGY; TEM; VISUALIZATION AB Lithium ion batteries are the dominant form of energy storage in mobile devices, increasingly employed in transportation, and likely candidates for renewable energy storage and integration into the electrical grid. To fulfil their powerful potential, electrodes with increased capacity, faster charge rates, and longer cycle life must be developed. Understanding the mechanics and chemistry of individual nanoparticles under in situ conditions is a crucial step to improving performance and mitigating damage. Here we reveal three-dimensional strain evolution within a single nanoparticle of a promising high voltage cathode material, LiNi0.5Mn1.5O4, under in situ conditions. The particle becomes disconnected during the second charging cycle. This is attributed to the formation of a cathode electrolyte interphase layer with slow ionic conduction. The three-dimensional strain pattern within the particle is independent of cell voltage after disconnection, indicating that the particle is unable to redistribute lithium within its volume or to its neighbours. Understanding the disconnection process at the single particle level and the equilibrium or non-equilibrium state of nanoparticles is essential to improving performance of current and future electrochemical energy storage systems. C1 [Ulvestad, Andrew; Singer, Andrej; Shpyrko, Oleg G.] Univ Calif San Diego, Dept Phys, La Jolla, CA 92093 USA. [Clark, Jesse N.] SLAC Natl Accelerator Lab, Stanford PULSE Inst, Menlo Pk, CA 94025 USA. [Clark, Jesse N.] DESY, Ctr Free Electron Laser Sci CFEL, D-22607 Hamburg, Germany. [Vine, David; Harder, Ross] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. [Cho, H. M.; Meng, Ying Shirley] Univ Calif San Diego, Dept NanoEngn, La Jolla, CA 92093 USA. RP Ulvestad, A (reprint author), Univ Calif San Diego, Dept Phys, La Jolla, CA 92093 USA. EM andrew.ulvestad@gmail.com RI Ulvestad, Andrew/K-8888-2015; Singer, Andrej/M-3948-2015 OI Ulvestad, Andrew/0000-0003-4611-2561; FU U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001805]; U.S. Department of Energy, Office of Basic Energy Sciences [DE-SC0002357]; U.S. D.O.E. [DE-AC02-06CH11357]; Volkswagen Foundation FX This work was supported by U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract DE-SC0001805. H.M.C. and Y.S.M. acknowledge the financial support by U.S. Department of Energy, Office of Basic Energy Sciences, under Award Number DE-SC0002357. O.G.S. and Y.S.M. are grateful to the UCSD Chancellor's Interdisciplinary Collaborators Award that made this collaboration possible. 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. D.O.E. under Contract No. DE-AC02-06CH11357. A.U. thanks the staff at Argonne National Laboratory and the Advanced Photon Source for their support. J.N.C gratefully acknowledges financial support from the Volkswagen Foundation. NR 42 TC 5 Z9 5 U1 9 U2 35 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2015 VL 17 IS 16 BP 10551 EP 10555 DI 10.1039/c5cp00372e PG 5 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA CF7AB UT WOS:000352707200027 PM 25804979 ER PT J AU Zhou, TY Qi, QY Zhao, QL Fu, J Liu, Y Ma, Z Zhao, X AF Zhou, Tian-You Qi, Qiao-Yan Zhao, Qiao-Ling Fu, Jie Liu, Yi Ma, Zhi Zhao, Xin TI Highly thermally stable hydrogels derived from monolayered two-dimensional supramolecular polymers SO POLYMER CHEMISTRY LA English DT Article ID HOST-GUEST INTERACTIONS; IN-VIVO; WATER; PHOTOCYCLODIMERIZATION; POLYMERIZATION; STOICHIOMETRY; CYCLODEXTRIN; CUCURBITURIL; CHEMISTRY; COPOLYMER AB It has been predicted that the properties of materials are dramatically influenced if their structures are confined to two-dimensional (2D) space. A representative example is graphene. However, for synthetic 2D materials, such influences have rarely been demonstrated. In this work, a rare example of how a 2D monolayer structure can impact the properties of bulk materials has been demonstrated by the construction of 2D supramolecular polymers (SPs) and their utilization in the fabrication of hydrogels. Maintaining the intrinsic 2D structures, the as-prepared hydrogels exhibited exceptional thermal stabilities (>180 degrees C), as revealed by an inversion test and a variable-temperature rheological study. The microstructures and morphologies of the 2D SPs have been extensively characterized by NMR spectroscopy, dynamic light scattering, small-angel X-ray scattering, transmission electron microscopy and atomic force microscopy. Furthermore, molecular dynamic simulations were also performed to shed light on the formation mechanism of the hydrogels. C1 [Zhou, Tian-You; Qi, Qiao-Yan; Zhao, Qiao-Ling; Fu, Jie; Ma, Zhi; Zhao, Xin] Chinese Acad Sci, Shanghai Inst Organ Chem, Key Lab Synthet & Self Assembly Chem Organ Funct, Shanghai 200032, Peoples R China. [Liu, Yi] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA. RP Zhao, X (reprint author), Chinese Acad Sci, Shanghai Inst Organ Chem, Key Lab Synthet & Self Assembly Chem Organ Funct, 345 Lingling Rd, Shanghai 200032, Peoples R China. EM xzhao@mail.sioc.ac.cn RI Liu, yi/A-3384-2008; Foundry, Molecular/G-9968-2014 OI Liu, yi/0000-0002-3954-6102; FU National Natural Science Foundation of China [21172249, 91127007]; Molecular Foundry, Lawrence Berkeley National Laboratory - Office of Science, Office of Basic Energy Sciences, Scientific User Facilities Division, of the U.S. Department of Energy [DE-AC02-05CH11231] FX We thank the National Natural Science Foundation of China (nos. 21172249 and 91127007) for financial support. Y.L. acknowledges the support from the Molecular Foundry, Lawrence Berkeley National Laboratory, supported by the Office of Science, Office of Basic Energy Sciences, Scientific User Facilities Division, of the U.S. Department of Energy under Contract no. DE-AC02-05CH11231. We also thank Prof. Zhan-Ting Li and Mr Jia Tian (Fudan University) for their help in preparing the manuscript and Prof. Li-Zhu Wu (Technical Institute of Physics and Chemistry) for her helpful advice. NR 48 TC 10 Z9 10 U1 3 U2 29 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1759-9954 EI 1759-9962 J9 POLYM CHEM-UK JI Polym. Chem. PY 2015 VL 6 IS 16 BP 3018 EP 3023 DI 10.1039/c5py00072f PG 6 WC Polymer Science SC Polymer Science GA CF6AV UT WOS:000352639700004 ER PT J AU Chapuis, G Le Boudic-Jamin, M Andonov, R Djidjev, H Lavenier, D AF Chapuis, Guillaume Le Boudic-Jamin, Mathilde Andonov, Rumen Djidjev, Hristo Lavenier, Dominique TI Parallel Seed-Based Approach to Multiple Protein Structure Similarities Detection SO SCIENTIFIC PROGRAMMING LA English DT Article ID STRUCTURE ALIGNMENT; MAXIMUM CLIQUES; ALGORITHM; SEQUENCE; QUALITY; GRAPHS AB Finding similarities between protein structures is a crucial task in molecular biology. Most of the existing tools require proteins to be aligned in order-preserving way and only find single alignments even when multiple similar regions exist. We propose a new seed-based approach that discovers multiple pairs of similar regions. Its computational complexity is polynomial and it comes with a quality guarantee-the returned alignments have both root mean squared deviations (coordinate-based as well as internal-distances based) lower than a given threshold, if such exist. We do not require the alignments to be order preserving (i.e., we consider nonsequential alignments), which makes our algorithm suitable for detecting similar domains when comparing multidomain proteins as well as to detect structural repetitions within a single protein. Because the search space for nonsequential alignments is much larger than for sequential ones, the computational burden is addressed by extensive use of parallel computing techniques: a coarse-grain level parallelism making use of available CPU cores for computation and a fine-grain level parallelism exploiting bit-level concurrency as well as vector instructions. C1 [Chapuis, Guillaume; Le Boudic-Jamin, Mathilde; Andonov, Rumen; Lavenier, Dominique] INRIA IRISA, F-35042 Rennes, France. [Chapuis, Guillaume; Le Boudic-Jamin, Mathilde; Andonov, Rumen; Lavenier, Dominique] Univ Rennes 1, F-35042 Rennes, France. [Djidjev, Hristo] Los Alamos Natl Lab, Informat Sci, Los Alamos, NM 87545 USA. RP Andonov, R (reprint author), INRIA IRISA, Campus Univ Beaulieu, F-35042 Rennes, France. EM rumen.andonov@irisa.fr NR 34 TC 0 Z9 0 U1 1 U2 3 PU HINDAWI PUBLISHING CORP PI NEW YORK PA 410 PARK AVENUE, 15TH FLOOR, #287 PMB, NEW YORK, NY 10022 USA SN 1058-9244 EI 1875-919X J9 SCI PROGRAMMING-NETH JI Sci. Program. PY 2015 AR 279715 DI 10.1155/2015/279715 PG 12 WC Computer Science, Software Engineering SC Computer Science GA CF9VJ UT WOS:000352915000001 ER PT J AU Momin, N Lee, S Gadok, AK Busch, DJ Bachand, GD Hayden, CC Stachowiak, JC Sasaki, DY AF Momin, Noor Lee, Stacey Gadok, Avinash K. Busch, David J. Bachand, George D. Hayden, Carl C. Stachowiak, Jeanne C. Sasaki, Darryl Y. TI Designing lipids for selective partitioning into liquid ordered membrane domains SO SOFT MATTER LA English DT Article ID AIR-WATER-INTERFACE; POLY(ETHYLENE GLYCOL); PHASE-SEPARATION; MODEL MEMBRANES; MIXED MONOLAYERS; PROTEINS; VESICLES; RAFTS; BEHAVIOR; PACKING AB Self-organization of lipid molecules into specific membrane phases is key to the development of hierarchical molecular assemblies that mimic cellular structures. While the packing interaction of the lipid tails should provide the major driving force to direct lipid partitioning to ordered or disordered membrane domains, numerous examples show that the headgroup and spacer play important but undefined roles. We report here the development of several new biotinylated lipids that examine the role of spacer chemistry and structure on membrane phase partitioning. The new lipids were prepared with varying lengths of low molecular weight polyethylene glycol (EGn) spacers to examine how spacer hydrophilicity and length influence their partitioning behavior following binding with FITC-labeled streptavidin in liquid ordered (L-o) and liquid disordered (L-d) phase coexisting membranes. Partitioning coefficients (K-p L-o/L-d) of the biotinylated lipids were determined using fluorescence measurements in studies with giant unilamellar vesicles (GUVs). Compared against DPPE-biotin, DPPE-cap-biotin, and DSPE-PEG2000-biotin lipids, the new dipalmityl-EGn-biotin lipids exhibited markedly enhanced partitioning into liquid ordered domains, achieving K-p of up to 7.3 with a decaethylene glycol spacer (DP-EG10-biotin). We further demonstrated biological relevance of the lipids with selective partitioning to lipid raft-like domains observed in giant plasma membrane vesicles (GPMVs) derived from mammalian cells. Our results found that the spacer group not only plays a pivotal role for designing lipids with phase selectivity but may also influence the structural order of the domain assemblies. C1 [Momin, Noor; Lee, Stacey; Sasaki, Darryl Y.] Sandia Natl Labs, Biotechnol & Bioengn Dept, Livermore, CA 94550 USA. [Hayden, Carl C.] Sandia Natl Labs, Combust Chem Dept, Livermore, CA USA. [Bachand, George D.] Sandia Natl Labs, Nanosyst Synth Anal Dept, Albuquerque, NM 87185 USA. [Momin, Noor; Gadok, Avinash K.; Busch, David J.; Stachowiak, Jeanne C.] Univ Texas Austin, Dept Biomed Engn, Austin, TX 78712 USA. RP Sasaki, DY (reprint author), Sandia Natl Labs, Biotechnol & Bioengn Dept, Livermore, CA 94550 USA. EM dysasak@sandia.gov OI Bachand, George/0000-0002-3169-9980 FU US Department of Energy, Office of Basic Energy Sciences, Materials Science and Engineering Division [KC0203010]; National Science Foundation, Division of Materials Research [DMR-1352487]; U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX The authors would like to thank Ms April Nissen for conducting the DSC measurements on the lipids and Prof. Paul Cremer (Pennsylvania State University) and Profs. Marjorie Longo and Tonya Kuhl (UC Davis) for their insightful discussions. This work was supported by the US Department of Energy, Office of Basic Energy Sciences, Materials Science and Engineering Division (KC0203010). GPMV studies were performed by AKG and DJB. JCS acknowledges support from the National Science Foundation, Division of Materials Research under grant DMR-1352487. 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 49 TC 5 Z9 5 U1 7 U2 31 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1744-683X EI 1744-6848 J9 SOFT MATTER JI Soft Matter PY 2015 VL 11 IS 16 BP 3241 EP 3250 DI 10.1039/c4sm02856b PG 10 WC Chemistry, Physical; Materials Science, Multidisciplinary; Physics, Multidisciplinary; Polymer Science SC Chemistry; Materials Science; Physics; Polymer Science GA CF8DD UT WOS:000352784900017 PM 25772372 ER PT S AU Ginocchio, JN AF Ginocchio, Joseph N. BE Gargano, A Coraggio, L Itaco, N TI Pseudospin Dynamical Symmetry in Nuclei SO 11TH INTERNATIONAL SPRING SEMINAR ON NUCLEAR PHYSICS: SHELL MODEL AND NUCLEAR STRUCTURE - ACHIEVEMENTS OF THE PAST TWO DECADES SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 11th International Spring Seminar on Nuclear Physics - Shell Model and Nuclear Structure - Achievements of the Past Two Decades CY MAY 12-16, 2014 CL Ischia, ITALY SP Dipartimento Fisica, Ist Nazl Fisica Nucleare, Univ Naples Federico II ID RELATIVISTIC SYMMETRY; TRANSITIONS AB Pseudospin symmetry has been useful in understanding atomic nuclei. We review the arguments that this symmetry is a relativistic symmetry. The condition for this symmetry is that the sum of the vector and scalar potentials in the Dirac Hamiltonian is a constant. We give the generators of pseudospin symmetry. We review some of the predictions that follow from this insight into the relativistic origins of pseudospin symmetry. Since in nuclei the sum of the scalar and vector potentials is not zero but is small, we discuss preliminary investigations into the conditions on the potentials to produce partial dynamic pseudospin symmetry. Finally we show that approximate pseudospin symmetry in nuclei predicts approximate spin symmetry in anti-nucleon scattering from nuclei. C1 Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Ginocchio, JN (reprint author), Los Alamos Natl Lab, MS 283, Los Alamos, NM 87545 USA. EM gino@lanl.gov NR 24 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 2015 VL 580 AR 012036 DI 10.1088/1742-6596/580/1/012036 PG 6 WC Physics, Multidisciplinary; Physics, Nuclear SC Physics GA BC3ZO UT WOS:000352130800036 ER PT S AU Iskra, LW Broda, R Janssens, RVF Wrzesinski, J Szpak, B Chiara, CJ Carpenter, MP Fornal, B Hoteling, N Kondev, FG Krolas, W Lauritsen, T Pawlat, T Seweryniak, D Stefanescu, I Walters, WB Zhu, S AF Iskra, L. W. Broda, R. Janssens, R. V. F. Wrzesinski, J. Szpak, B. Chiara, C. J. Carpenter, M. P. Fornal, B. Hoteling, N. Kondev, F. G. Krolas, W. Lauritsen, T. Pawlat, T. Seweryniak, D. Stefanescu, I. Walters, W. B. Zhu, S. BE Gargano, A Coraggio, L Itaco, N TI High-spin shell model states in neutron-rich Sn isotopes SO 11TH INTERNATIONAL SPRING SEMINAR ON NUCLEAR PHYSICS: SHELL MODEL AND NUCLEAR STRUCTURE - ACHIEVEMENTS OF THE PAST TWO DECADES SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 11th International Spring Seminar on Nuclear Physics - Shell Model and Nuclear Structure - Achievements of the Past Two Decades CY MAY 12-16, 2014 CL Ischia, ITALY SP Dipartimento Fisica, Ist Nazl Fisica Nucleare, Univ Naples Federico II ID HEAVY-ION COLLISIONS; YRAST ISOMERS; NUCLEI; SUBSHELL AB High-spin states with the seniority nu >= 2 have been investigated in the neutron-rich Sn-118,Sn-120,Sn-122,Sn-124,Sn-126 isotopes. They were produced in fusion-fission processes following Ca-48 + Pb-208, Ca-48 + U-238 reactions and via fission of target nuclei in the Ni-64 + U-238 system. By employing techniques of delayed-and cross-coincidences, it was possible to establish level schemes up to an 8 MeV excitation energy. The 13(-) and 15(-) states were identified as being isomeric and their half-lives were determined. The reduced transition probabilities extracted for isomeric transitions behave very regularly with the mass number A. The spin-parity values assigned to or suggested for the identified states were supported by shell-model calculations and by systematics. C1 [Iskra, L. W.; Broda, R.; Wrzesinski, J.; Szpak, B.; Fornal, B.; Krolas, W.; Pawlat, T.] Polish Acad Sci, Inst Nucl Phys, PL-31342 Krakow, Poland. [Janssens, R. V. F.; Chiara, C. J.; Carpenter, M. P.; Hoteling, N.; Lauritsen, T.; Seweryniak, D.; Stefanescu, I.; Zhu, S.] Argonne Natl Lab, Div Phys, Argonne, IL 60439 USA. [Chiara, C. J.; Hoteling, N.; Stefanescu, I.; Walters, W. B.] Univ Maryland, Dept Chem & Biochem, College Pk, MD 20742 USA. [Kondev, F. G.] Argonne Natl Lab, Nucl Engn Div, Argonne, IL 60439 USA. RP Iskra, LW (reprint author), Polish Acad Sci, Inst Nucl Phys, PL-31342 Krakow, Poland. EM lukasz.iskra@ifj.edu.pI RI Carpenter, Michael/E-4287-2015 OI Carpenter, Michael/0000-0002-3237-5734 NR 17 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 2015 VL 580 AR 012037 DI 10.1088/1742-6596/580/1/012037 PG 6 WC Physics, Multidisciplinary; Physics, Nuclear SC Physics GA BC3ZO UT WOS:000352130800037 ER PT S AU Moretto, LG Larsen, AC Giacoppo, F Guttormsen, M Siem, S AF Moretto, L. G. Larsen, A. C. Giacoppo, F. Guttormsen, M. Siem, S. BE Gargano, A Coraggio, L Itaco, N TI Experimental First Order Pairing Phase Transition in Atomic Nuclei SO 11TH INTERNATIONAL SPRING SEMINAR ON NUCLEAR PHYSICS: SHELL MODEL AND NUCLEAR STRUCTURE - ACHIEVEMENTS OF THE PAST TWO DECADES SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 11th International Spring Seminar on Nuclear Physics - Shell Model and Nuclear Structure - Achievements of the Past Two Decades CY MAY 12-16, 2014 CL Ischia, ITALY SP Dipartimento Fisica, Ist Nazl Fisica Nucleare, Univ Naples Federico II AB The natural log of experimental nuclear level densities at low energy is linear with energy. This can be interpreted in terms of a nearly 1st order phase transition from a superfluid to an ideal gas of quasi particles. The transition temperature coincides with the BCS critical temperature and yields gap parameters in good agreement with the values extracted from evenodd mass differences from rotational states. This converging evidence supports the relevance of the BCS theory to atomic nuclei. C1 [Moretto, L. G.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Moretto, L. G.] Univ Calif Berkeley, Berkeley, CA 94720 USA. [Larsen, A. C.; Giacoppo, F.; Guttormsen, M.; Siem, S.] Univ Oslo, Dept Phys, N-0316 Oslo, Norway. RP Moretto, LG (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. EM lgmoretto@lbl.gov RI Larsen, Ann-Cecilie/C-8742-2014 OI Larsen, Ann-Cecilie/0000-0002-2188-3709 NR 17 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 2015 VL 580 AR 012048 DI 10.1088/1742-6596/580/1/012048 PG 6 WC Physics, Multidisciplinary; Physics, Nuclear SC Physics GA BC3ZO UT WOS:000352130800048 ER PT S AU Oganessian, YT Abdullin, FS Alexander, C Binder, J Boll, RA Dmitriev, SN Ezold, J Felker, K Gostic, JM Grzywacz, RK Hamilton, JH Henderson, RA Itkis, MG Miernik, K Miller, D Moody, KJ Polyakov, AN Ramayya, AV Roberto, JB Ryabinin, MA Rykaczewski, KP Sagaidak, RN Shaughnessy, DA Shirokovsky, IV Shumeiko, MV Stoyer, MA Stoyer, NJ Subbotin, VG Sukhov, AM Tsyganov, YS Utyonkov, VK Voinov, AA Vostokin, GK AF Oganessian, Yu Ts Abdullin, F. Sh Alexander, C. Binder, J. Boll, R. A. Dmitriev, S. N. Ezold, J. Felker, K. Gostic, J. M. Grzywacz, R. K. Hamilton, J. H. Henderson, R. A. Itkis, M. G. Miernik, K. Miller, D. Moody, K. J. Polyakov, A. N. Ramayya, A. V. Roberto, J. B. Ryabinin, M. A. Rykaczewski, K. P. Sagaidak, R. N. Shaughnessy, D. A. Shirokovsky, I. V. Shumeiko, M. V. Stoyer, M. A. Stoyer, N. J. Subbotin, V. G. Sukhov, A. M. Tsyganov, Yu S. Utyonkov, V. K. Voinov, A. A. Vostokin, G. K. BE Gargano, A Coraggio, L Itaco, N TI Production and decay of the heaviest odd-Z nuclei in the Bk-249+Ca-48 reaction SO 11TH INTERNATIONAL SPRING SEMINAR ON NUCLEAR PHYSICS: SHELL MODEL AND NUCLEAR STRUCTURE - ACHIEVEMENTS OF THE PAST TWO DECADES SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 11th International Spring Seminar on Nuclear Physics - Shell Model and Nuclear Structure - Achievements of the Past Two Decades CY MAY 12-16, 2014 CL Ischia, ITALY SP Dipartimento Fisica, Ist Nazl Fisica Nucleare, Univ Naples Federico II ID CHEMICAL-IDENTIFICATION; ELEMENT-115; DUBNIUM AB The reaction of Bk-249 with Ca-48 has been investigated with an aim of synthesizing and studying the decay properties of isotopes of the new element 117. The experiments were performed at five projectile energies (in two runs, in 2009-2010 and 2012) and with a total beam dose of Ca-48 ions of about 9x10(19). The experiments yielded data on alpha-decay characteristics and excitation functions of the produced nuclei that establish these to be (293)117 and (294)117 - the products of the 4n-and 3n-evaporation channels, respectively. In total, we have observed 20 decay chains of Z= 117 nuclides. The cross sections were measured to be 1.1 pb for the 3n and 2.4 pb for the 4n-reaction channel. The new (289)115 events, populated by a decay of (293)117, demonstrate the same decay properties as those observed for (289)115 produced in the Am-243(Ca-48, 2n) reaction thus providing cross-bombardment evidence. In addition, a single decay of (294)118 was observed from the reaction with Cf-249 -a result of the in-growth of Cf-249 in the Bk-249 target. The observed decay chain of (294)118 is in good agreement with decay properties obtained in 2002-2005 in the experiments with the reaction Cf-249(Ca-48, 3n) (294)118. The energies and half-lives of the odd-Z isotopes observed in the 117 decay chains together with the results obtained for lower-Z superheavy nuclei demonstrate enhancement of nuclear stability with increasing neutron number towards the predicted new magic number N= 184. C1 [Oganessian, Yu Ts; Abdullin, F. Sh; Dmitriev, S. N.; Itkis, M. G.; Polyakov, A. N.; Sagaidak, R. N.; Shirokovsky, I. V.; Shumeiko, M. V.; Subbotin, V. G.; Sukhov, A. M.; Tsyganov, Yu S.; Utyonkov, V. K.; Voinov, A. A.; Vostokin, G. K.] Joint Inst Nucl Res, RU-141980 Dubna, Russia. [Alexander, C.; Binder, J.; Boll, R. A.; Ezold, J.; Felker, K.; Grzywacz, R. K.; Miernik, K.; Roberto, J. B.; Rykaczewski, K. P.] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. [Gostic, J. M.; Henderson, R. A.; Moody, K. J.; Shaughnessy, D. A.; Stoyer, M. A.; Stoyer, N. J.] Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. [Grzywacz, R. K.; Miller, D.] Univ Tennessee, Knoxville, TN 37996 USA. [Hamilton, J. H.; Ramayya, A. V.] Vanderbilt Univ, Nashville, TN 37235 USA. [Ryabinin, M. A.] Res Inst Atom Reactors, RU-433510 Dimitrovgrad, Russia. RP Oganessian, YT (reprint author), Joint Inst Nucl Res, RU-141980 Dubna, Russia. EM voinov_2000@mail.ru RI Boll, Rose/C-4138-2016; OI Boll, Rose/0000-0003-2507-4834; Ezold, Julie/0000-0002-5055-0022; Roberto, James/0000-0002-4234-0252 NR 26 TC 2 Z9 2 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 2015 VL 580 AR 012038 DI 10.1088/1742-6596/580/1/012038 PG 6 WC Physics, Multidisciplinary; Physics, Nuclear SC Physics GA BC3ZO UT WOS:000352130800038 ER PT S AU Podolyak, Z Shand, CM Wilson, E Brown, BA Grawe, H Chiara, CJ Zhu, S Fornal, B Janssens, RVF Bowry, M Bunce, M Carpenter, MP Cieplicka, N Deo, AY Dracoulis, GD Hoffman, CR Kempley, RS Kondev, FG Lane, GJ Lauritsen, T Lotay, G Reed, MW Regan, PH Triguero, CR Seweryniak, D Szpak, B Walker, PM AF Podolyak, Zs Shand, C. M. Wilson, E. Brown, B. A. Grawe, H. Chiara, C. J. Zhu, S. Fornal, B. Janssens, R. V. F. Bowry, M. Bunce, M. Carpenter, M. P. Cieplicka, N. Deo, A. Y. Dracoulis, G. D. Hoffman, C. R. Kempley, R. S. Kondev, F. G. Lane, G. J. Lauritsen, T. Lotay, G. Reed, M. W. Regan, P. H. Triguero, C. Rodriguez Seweryniak, D. Szpak, B. Walker, P. M. BE Gargano, A Coraggio, L Itaco, N TI Octupole transitions in the Pb-208 region SO 11TH INTERNATIONAL SPRING SEMINAR ON NUCLEAR PHYSICS: SHELL MODEL AND NUCLEAR STRUCTURE - ACHIEVEMENTS OF THE PAST TWO DECADES SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 11th International Spring Seminar on Nuclear Physics - Shell Model and Nuclear Structure - Achievements of the Past Two Decades CY MAY 12-16, 2014 CL Ischia, ITALY SP Dipartimento Fisica, Ist Nazl Fisica Nucleare, Univ Naples Federico II ID NUCLEAR-DATA SHEETS AB The Pb-208 region is characterised by the existence of collective octupole states. Here we populated such states in (208)pb + (208)pb deep-inelastic reactions. gamma-ray angular distribution measurements were used to infer the octupole character of several E3 transitions. The octupole character of the 2318 keV 17(-) 14(+) in (208)bp D 2485 keV 19/2(-) -> 13/2(+) in Pb-207, D 2419 keV 15/2(-) -> 9/2(+) in Pb-209 and 2465 keV 17/2(+) -> 11/2(-) in (TI)-T-207 transitions was demonstrated for the first time. In addition, shell model calculations were performed using two different sets of two-body matrix elements. Their predictions were compared with emphasis on collective octupole states. C1 [Podolyak, Zs; Shand, C. M.; Wilson, E.; Bowry, M.; Bunce, M.; Kempley, R. S.; Lotay, G.; Regan, P. H.; Walker, P. M.] Univ Surrey, Dept Phys, Guildford GU2 7XH, Surrey, England. [Brown, B. A.] Michigan State Univ, E Lansing, MI 48824 USA. [Grawe, H.] GSI Helmholtzzentrum Schwerionenforsch GmbH, D-64291 Darmstadt, Germany. [Chiara, C. J.; Zhu, S.; Janssens, R. V. F.; Carpenter, M. P.; Hoffman, C. R.; Lauritsen, T.; Seweryniak, D.] Argonne Natl Lab, Div Phys, Argonne, IL 60439 USA. [Chiara, C. J.] Univ Maryland, Dept Chem & Biochem, College Pk, MD 20742 USA. [Fornal, B.; Cieplicka, N.; Szpak, B.] H Niewodniczanski Inst Nucl Phys, PL-31342 Krakow, Poland. [Deo, A. Y.] Univ Massachusetts, Dept Phys, Lowell, MA 01854 USA. [Deo, A. Y.] Indian Inst Technol, Dept Phys, Roorkee 247667, Uttar Pradesh, India. [Dracoulis, G. D.; Lane, G. J.; Reed, M. W.] Australian Natl Univ, Res Sch Phys & Engn, Dept Nucl Phys, Canberra, ACT 0200, Australia. [Kondev, F. G.] Argonne Natl Lab, Nucl Engn Div, Argonne, IL 60439 USA. [Regan, P. H.] Natl Phys Lab, Teddington TW11 0LW, Middx, England. [Triguero, C. Rodriguez] Univ Brighton, Sch Comp Engn & Math, Brighton BN2 4GL, E Sussex, England. RP Podolyak, Z (reprint author), Univ Surrey, Dept Phys, Guildford GU2 7XH, Surrey, England. EM z.podolyak@surrey.ac.uk RI Carpenter, Michael/E-4287-2015; Lane, Gregory/A-7570-2011; OI Carpenter, Michael/0000-0002-3237-5734; Lane, Gregory/0000-0003-2244-182X; Wilson, Emma/0000-0003-2695-9853 NR 25 TC 3 Z9 3 U1 6 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 2015 VL 580 AR 012010 DI 10.1088/1742-6596/580/1/012010 PG 6 WC Physics, Multidisciplinary; Physics, Nuclear SC Physics GA BC3ZO UT WOS:000352130800010 ER PT S AU Frisch, PC Berdyugin, A Funsten, HO Magalhaes, AM McComas, DJ Piirola, V Schwadron, NA Seriacopi, DB Wiktorowicz, SJ AF Frisch, P. C. Berdyugin, A. Funsten, H. O. Magalhaes, A. M. McComas, D. J. Piirola, V. Schwadron, N. A. Seriacopi, D. B. Wiktorowicz, S. J. BE Zank, GP TI Connecting the interstellar magnetic field at the heliosphere to the Loop I superbubble SO 13TH ANNUAL INTERNATIONAL ASTROPHYSICS CONFERENCE: VOYAGER, IBEX, AND THE INTERSTELLAR MEDIUM SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 13th Annual International Astrophysics Conference on Voyager, IBEX, and the Interstellar Medium CY MAR 10-14, 2014 CL Myrtle Beach, SC ID NORTH POLAR SPUR; BOUNDARY-EXPLORER RIBBON; ENERGETIC NEUTRAL ATOMS; GALACTIC ENVIRONMENT; SCORPIO-CENTAURUS; LOCAL BUBBLE; IBEX; POLARIZATION; STARS; SUN AB The local interstellar magnetic field affects both the heliosphere and the surrounding cluster of interstellar clouds (CLIC). Measurements of linearly polarized starlight provide the only test of the magnetic field threading the CLIC. Polarization measurements of the CLIC magnetic field show multiple local magnetic structures, one of which is aligned with the magnetic field traced by the center of the "ribbon" of energetic neutral atoms discovered by the Interstellar Boundary Explorer (IBEX). Comparisons between the bulk motion of the CLIC through the local standard of rest, the magnetic field direction, the geometric center of Loop I, and the polarized dust bridge extending from the heliosphere toward the North Polar Spur direction all suggest that the CLIC is part of the rim region of the Loop I superbubble. C1 [Frisch, P. C.] Univ Chicago, Dept Astron & Astrophys, Chicago, IL 60637 USA. [Berdyugin, A.; Piirola, V.] Univ Turku, Finnish Ctr Astron ESO, SF-20500 Turku, Finland. [Funsten, H. O.] Los Alamos Natl Lab, Los Alamos, NM USA. [Magalhaes, A. M.; Seriacopi, D. B.] Univ Sao Paulo, Inst Astron Geofis & Ciencias Atmosfer, BR-05508 Sao Paulo, Brazil. [McComas, D. J.] Southwest Res Inst, San Antonio, TX USA. [McComas, D. J.] Univ Texas San Antonio, San Antonio, TX USA. [Schwadron, N. A.] Univ New Hampshire, Ctr Space Sci, Durham, NH 03824 USA. [Wiktorowicz, S. J.] Univ Calif Santa Cruz, Dept Astron, Santa Cruz, CA 95064 USA. RP Frisch, PC (reprint author), Univ Chicago, Dept Astron & Astrophys, 5640 S Ellis Ave, Chicago, IL 60637 USA. EM frisch@oddjob.uchicago.edu OI Funsten, Herbert/0000-0002-6817-1039 NR 59 TC 4 Z9 4 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 2015 VL 577 AR 012010 DI 10.1088/1742-6596/577/1/012010 PG 10 WC Astronomy & Astrophysics SC Astronomy & Astrophysics GA BC3YZ UT WOS:000352101600010 ER PT S AU Schwadron, NA Adams, FC Christian, E Desiati, P Frisch, P Funsten, HO Jokipii, JR McComas, DJ Moebius, E Zank, GP AF Schwadron, N. A. Adams, F. C. Christian, E. Desiati, P. Frisch, P. Funsten, H. O. Jokipii, J. R. McComas, D. J. Moebius, E. Zank, G. P. BE Zank, GP TI Anisotropies in TeV Cosmic Rays Related to the Local Interstellar Magnetic Field from the IBEX Ribbon SO 13TH ANNUAL INTERNATIONAL ASTROPHYSICS CONFERENCE: VOYAGER, IBEX, AND THE INTERSTELLAR MEDIUM SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 13th Annual International Astrophysics Conference on Voyager, IBEX, and the Interstellar Medium CY MAR 10-14, 2014 CL Myrtle Beach, SC ID BOUNDARY-EXPLORER RIBBON; ARRIVAL DIRECTIONS; LO OBSERVATIONS; ENA FLUX; CLOUD; SCINTILLATION; HELIOSPHERE; SPECTRUM; ICECUBE; SIRIUS AB The Interstellar Boundary Explorer (IBEX) observes enhanced Energetic Neutral Atoms (ENAs) emission in the keV energy range from a narrow (similar to 20 degrees wide) "ribbon" in the sky that appears to be centered on the direction of the local interstellar (LIS) magnetic field. The Milagro collaboration, the As gamma collaboration and the Ice Cube observatory have recently made global maps of cosmic ray fluxes in the TeV energy range, revealing anisotropic structures ordered in part by the local interstellar magnetic field and the interstellar flow. This paper following from a recent publication in Science makes the link between these disparate observations by developing a simple model of the magnetic structure surrounding the heliosphere in the Local Interstellar Medium (LISM) that is consistent with both IBEX ENA fluxes and TeV cosmic ray anisotropies. The model also employs the revised velocity direction of the LIC derived from neutral He observations by IBEX. By modeling the propagation of cosmic rays through this magnetic field structure, we specifically show that (1) the large-scale TeV anisotropy provides a roughly consistent orientation for the local interstellar magnetic field at the center of the IBEX Ribbon and corroborates the 3,uG magnitude of the local interstellar magnetic field derived from IBEX observations of the global heliosphere; (2) and small-scale structures in cosmic rays (over < 30 angular scales) are influenced by the interstellar field interaction with the heliosphere at energies < 10 TeV. Thus, we provide a link between IBEX ENA observations, IBEX neutral observations of interstellar He, and TeV cosmic ray anisotropies, which are strongly influenced by the interactions between the local interstellar magnetic field, the flow of the local interstellar plasma, and the global heliosphere. C1 [Schwadron, N. A.; Moebius, E.] Univ New Hampshire, Durham, NH 03824 USA. [Schwadron, N. A.; McComas, D. J.] SW Res Inst, San Antonio, TX 78228 USA. [Adams, F. C.] Univ Michigan, Ann Arbor, MI 48109 USA. [Christian, E.] NASA, Goddard Space Flight Ctr, Greenbelt, MD 20771 USA. [Frisch, P.] Univ Wisconsin, IceCube Res Ctr, Madison, WI 53706 USA. [Desiati, P.] Univ Wisconsin, Dept Astron, Madison, WI 53706 USA. [Frisch, P.] Univ Chicago, Dept Astron & Astrophys, Chicago, IL 60637 USA. [Funsten, H. O.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Jokipii, J. R.] Univ Arizona, Dept Planetary Sci, Tucson, AZ 85721 USA. [McComas, D. J.] Univ Texas San Antonio, San Antonio, TX 78228 USA. [Zank, G. P.] Univ Alabama, Huntsville, AL 35805 USA. RP Schwadron, NA (reprint author), Univ New Hampshire, Durham, NH 03824 USA. EM n.schwadron@unh.edu OI Funsten, Herbert/0000-0002-6817-1039; Moebius, Eberhard/0000-0002-2745-6978 NR 34 TC 1 Z9 1 U1 0 U2 2 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2015 VL 577 AR 012023 DI 10.1088/1742-6596/577/1/012023 PG 11 WC Astronomy & Astrophysics SC Astronomy & Astrophysics GA BC3YZ UT WOS:000352101600023 ER PT S AU Lukishova, SG Winkler, JM Mihaylova, D Liapis, A Bissell, LJ Goldberg, D Menon, VM Shi, ZM Boyd, RW Chen, GN Prasad, P AF Lukishova, Svetlana G. Winkler, Justin M. Mihaylova, Dilyana Liapis, Andreas Bissell, Luke J. Goldberg, David Menon, Vinod M. Shi, Zhimin Boyd, Robert W. Chen, Guanuing Prasad, Paras GP IOP TI Nanocrystal fluorescence in photonic bandgap microcavities and plasmonic nanoantennas SO 23RD INTERNATIONAL LASER PHYSICS WORKSHOP (LPHYS'14) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 23rd International Laser Physics Workshop (LPHYS) CY JUL 14-18, 2014 CL Bulgarian Acad Sci, Inst Elect, Sofia, BULGARIA HO Bulgarian Acad Sci, Inst Elect ID LIQUID-CRYSTAL HOST; DYE MOLECULE FLUORESCENCE; SINGLE AB Results are presented here towards robust room-temperature single-photon sources based on fluorescence in nanocrystals: colloidal quantum dots, color-center diamonds and doped with trivalent rare-earth ions (TR3+). We used cholesteric chiral photonic bandgap and Bragg-reflector microcavities for single emitter fluorescence enhancement. We also developed plasmonic bowtie nanoantennas and 2D-Si-photonic bandgap microcavities. C1 [Lukishova, Svetlana G.; Mihaylova, Dilyana; Boyd, Robert W.] Univ Rochester, Inst Opt, Rochester, NY 14627 USA. [Winkler, Justin M.; Boyd, Robert W.] Univ Rochester, Dept Phys & Astron, Rochester, NY 14627 USA. [Liapis, Andreas] Brookhaven Natl Lab, Upton, NY 11973 USA. [Bissell, Luke J.] US Air Force, Res Lab, Wright Patterson AFB, OH 45433 USA. [Goldberg, David; Menon, Vinod M.] CUNY, Dept Phys, New York, NY 10031 USA. [Shi, Zhimin] Univ S Florida, Dept Phys, Tampa, FL 33620 USA. [Boyd, Robert W.] Univ Ottawa, Dept Phys, Ottawa, ON K1N 6N5, Canada. [Boyd, Robert W.] Univ Ottawa, Sch Elect Engn & Comp Sci, Ottawa, ON K1N 6N5, Canada. [Chen, Guanuing; Prasad, Paras] SUNY Buffalo, Inst Lasers Photon & Biophoton, Buffalo, NY 14260 USA. [Chen, Guanuing; Prasad, Paras] SUNY Buffalo, Dept Chem, Buffalo, NY 14260 USA. RP Lukishova, SG (reprint author), Univ Rochester, Inst Opt, Rochester, NY 14627 USA. EM sluk@lle.rochester.edu OI Liapis, Andreas/0000-0001-6810-3354 NR 31 TC 0 Z9 0 U1 2 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 2015 VL 594 AR 012005 DI 10.1088/1742-6596/594/1/012005 PG 10 WC Engineering, Electrical & Electronic; Optics; Physics, Applied SC Engineering; Optics; Physics GA BC3YJ UT WOS:000352084500004 ER PT J AU Loizides, C AF Loizides, C. TI First results on p-Pb collisions from ALICE SO ANNALS OF PHYSICS LA English DT Article DE Nuclear modification factor; Elliptic flow; Identified particles; Mean transverse momentum ID AVERAGE TRANSVERSE-MOMENTUM; RANGE ANGULAR-CORRELATIONS; COLOR GLASS CONDENSATE; LONG-RANGE; PLUS PB; MULTIPLICITY DEPENDENCE; CENTRALITY DEPENDENCE; ROOT-S(NN)=5.02 TEV; PPB COLLISIONS; LHC AB First results from p-Pb collisions at root S-NN = 5.02 TeV published by the ALICE collaboration till summer 2013 are summarized. Published by Elsevier Inc. C1 Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Nucl Sci, Berkeley, CA 94720 USA. RP Loizides, C (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Nucl Sci, Berkeley, CA 94720 USA. EM cloizides@lbl.gov NR 52 TC 1 Z9 1 U1 0 U2 3 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 0003-4916 EI 1096-035X J9 ANN PHYS-NEW YORK JI Ann. Phys. PD JAN PY 2015 VL 352 SI SI BP 41 EP 51 DI 10.1016/j.aop.2014.07.044 PG 11 WC Physics, Multidisciplinary SC Physics GA CE8VS UT WOS:000352122800006 ER PT J AU McLerran, L AF McLerran, L. TI Lessons learned and ideas formed from early studies of pA collisions SO ANNALS OF PHYSICS LA English DT Article ID CHARGED-PARTICLE MULTIPLICITY; GLUON DISTRIBUTION-FUNCTIONS; NUCLEUS-NUCLEUS COLLISIONS; HIGH-ENERGIES; TRANSVERSE-MOMENTUM; PI AB I discuss ideas that were developed in the early studies of high energy proton nucleus collisions. (C) 2014 Elsevier Inc. All rights reserved. C1 [McLerran, L.] Brookhaven Natl Lab, Dept Phys, Upton, NY 11973 USA. [McLerran, L.] RIKEN, BNL Res Ctr, Brookhaven Natl Lab, Upton, NY 11973 USA. [McLerran, L.] Cent China Normal Univ, Dept Phys, Wuhan 430079, Peoples R China. RP McLerran, L (reprint author), Brookhaven Natl Lab, Dept Phys, Bdg 510A, Upton, NY 11973 USA. EM mclerran@mac.com FU DOE [DE-AC02-98CH10886] FX The research of L. McLerran is supported under DOE Contract No. DE-AC02-98CH10886. NR 15 TC 0 Z9 0 U1 0 U2 0 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 0003-4916 EI 1096-035X J9 ANN PHYS-NEW YORK JI Ann. Phys. PD JAN PY 2015 VL 352 SI SI BP 52 EP 58 DI 10.1016/j.aop.2014.07.036 PG 7 WC Physics, Multidisciplinary SC Physics GA CE8VS UT WOS:000352122800007 ER PT J AU Coleman-Smith, C Muller, B AF Coleman-Smith, Christopher Mueller, Berndt TI How to catch a 'fat' proton SO ANNALS OF PHYSICS LA English DT Article DE Proton; Fluctuation; Cross section ID ANTIQUARK DISTRIBUTIONS; PPB COLLISIONS; SCATTERING; NUCLEON; ASYMMETRY; LHC AB We argue that high-multiplicity events in proton proton or proton nucleus collisions originate from large-size fluctuations of the nucleon shape. We discuss a pair of simple models of such proton shape fluctuations. A "fat" proton with a size of 3 fm occurs with observable frequency. In light of this result, collective flow behavior in the ensuing nuclear interaction seems feasible. We discuss the influence of these models on the parton structure of the proton. (C) 2014 Elsevier Inc. All rights reserved. C1 [Coleman-Smith, Christopher; Mueller, Berndt] Duke Univ, Dept Phys, Durham, NC 27708 USA. [Mueller, Berndt] Brookhaven Natl Lab, Upton, NY 11973 USA. RP Muller, B (reprint author), Duke Univ, Dept Phys, Durham, NC 27708 USA. EM mueller@phy.duke.edu NR 30 TC 1 Z9 1 U1 0 U2 0 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 0003-4916 EI 1096-035X J9 ANN PHYS-NEW YORK JI Ann. Phys. PD JAN PY 2015 VL 352 SI SI BP 59 EP 69 DI 10.1016/j.aop.2014.07.040 PG 11 WC Physics, Multidisciplinary SC Physics GA CE8VS UT WOS:000352122800008 ER PT J AU Sickles, AM AF Sickles, Anne M. CA PHENIX Collaboration TI d plus Au hadron correlation measurements from PHENIX SO ANNALS OF PHYSICS LA English DT Article DE Heavy-ions ID ANGULAR-CORRELATIONS; PB COLLISIONS; TEV AB Recent observations of extended pseudorapidity correlations at the LHC in p + p and p + Pb collisions are of great interest. Here we present related results from d + Au collisions at PHENIX. We present the observed v(2) and discuss the possible origin in the geometry of the collision region. We also present new measurements of the pseudorapidity dependence of the ridge in d + Au collision. Future plans to clarify the role of geometry in small collision systems using He-3 + Au collisions are discussed. (C) 2014 Elsevier Inc. All rights reserved. C1 [Sickles, Anne M.; PHENIX Collaboration] Brookhaven Natl Lab, Dept Phys, Upton, NY 11973 USA. RP Sickles, AM (reprint author), Brookhaven Natl Lab, Dept Phys, Upton, NY 11973 USA. EM anne@bnl.gov NR 18 TC 0 Z9 0 U1 1 U2 2 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 0003-4916 EI 1096-035X J9 ANN PHYS-NEW YORK JI Ann. Phys. PD JAN PY 2015 VL 352 SI SI BP 78 EP 83 DI 10.1016/j.aop.2014.07.033 PG 6 WC Physics, Multidisciplinary SC Physics GA CE8VS UT WOS:000352122800010 ER PT J AU Steinberg, P AF Steinberg, Peter TI PHOBOS in the LHC era SO ANNALS OF PHYSICS LA English DT Article DE Heavy ion; Proton-nucleus; Deuteron-nucleus; Relativistic heavy-ion collider; Large hadron collider ID TRANSVERSE-MOMENTUM; PB COLLISIONS; DEPENDENCE; TEV AB The PHOBOS experiment ran at the RHIC collider from 2000 to 2005, under the leadership of Wit Busza. These proceedings summarize selected PHOBOS results, highlighting their continuing relevance amidst the wealth of new results from the lead-lead program at the Large Hadron Collider (LHC). (C) 2015 Published by Elsevier Inc. C1 Brookhaven Natl Lab, Upton, NY 11973 USA. RP Steinberg, P (reprint author), Brookhaven Natl Lab, Upton, NY 11973 USA. EM peter.steinberg@bnl.gov NR 37 TC 0 Z9 0 U1 0 U2 4 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 0003-4916 EI 1096-035X J9 ANN PHYS-NEW YORK JI Ann. Phys. PD JAN PY 2015 VL 352 SI SI BP 84 EP 95 DI 10.1016/j.aop.2014.07.042 PG 12 WC Physics, Multidisciplinary SC Physics GA CE8VS UT WOS:000352122800011 ER PT J AU Tannenbaum, MJ AF Tannenbaum, Michael J. TI Reminiscences of Wit Busza and 41 years of p plus A physics SO ANNALS OF PHYSICS LA English DT Article DE Experimental nuclear physics ID CHARGED-PARTICLE MULTIPLICITY; NUCLEUS-NUCLEUS COLLISIONS; CENTRAL RAPIDITY REGION; HEAVY-ION COLLISIONS; TRANSVERSE ENERGY; MULTIPARTICLE PRODUCTION; P+A COLLISIONS; AU COLLISIONS; 14.5 GEV/C; GEV-C AB One of the more memorable (and easiest) proposal to deal with when I served on Bob Wilson's Program Advisory Committee at NAL (Now Fermilab) from 1972 to 1975 was Proposal-178, "A study of the average multiplicity and multiplicity distributions in hadron-nucleus collisions at high energies", with only 4 authors, Wit Busza, Jerry Friedman, Henry Kendall and Larry Rosenson, as presented at the PAC meeting by Wit. What I remember was that he discussed only ONE, 5 inch photomultiplier with a Cherenkov radiator in the beam to make this measurement of production of charged particles with angles up to 30 degrees in various nuclei, 40 h requested. This turned out to be a "seminal" experiment leading to the Wounded Nucleon and other participant models. Subsequent p(d) + A experiments from the AGS to RHIC, as well as alpha-alpha measurements at the CERN-ISR, will be discussed together with the various 'participants' that they revealed. (C) 2014 Elsevier Inc. All rights reserved. C1 Brookhaven Natl Lab, Upton, NY 11973 USA. RP Tannenbaum, MJ (reprint author), Brookhaven Natl Lab, Upton, NY 11973 USA. EM mjt@bnl.gov OI Tannenbaum, Michael/0000-0002-8840-5314 FU US Department of Energy [DE-AC02-98CH10886] FX This research was supported by US Department of Energy, DE-AC02-98CH10886. NR 39 TC 0 Z9 0 U1 0 U2 1 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 0003-4916 EI 1096-035X J9 ANN PHYS-NEW YORK JI Ann. Phys. PD JAN PY 2015 VL 352 SI SI BP 96 EP 107 DI 10.1016/j.aop.2014.07.034 PG 12 WC Physics, Multidisciplinary SC Physics GA CE8VS UT WOS:000352122800012 ER PT J AU Venugopalan, R AF Venugopalan, Raju TI Long range correlations in high multiplicity hadron collisions: Building bridges with ridges SO ANNALS OF PHYSICS LA English DT Article DE Long range correlation; Multi particle production; QCD ID P-PB COLLISIONS; ANGULAR-CORRELATIONS; ION COLLISIONS; PPB COLLISIONS; SIDE; TEV AB We discuss the physics of the ridge - azimuthally collimated long range rapidity correlations - in high multiplicity proton-proton and proton-collisions. We outline some of the theoretical discussions in the literature that address the systematics of these ridge correlations. (C) 2014 Elsevier Inc. All rights reserved. C1 Brookhaven Natl Lab, Dept Phys, Upton, NY 11973 USA. RP Venugopalan, R (reprint author), Brookhaven Natl Lab, Dept Phys, Upton, NY 11973 USA. EM raju.venugopalan@gmail.com FU DOE [DE-AC02-98CH10886] FX R.V's research was supported by DOE Contract No. DE-AC02-98CH10886. He is grateful to James Bjorken, Adam Bzdak, Adrian Dumitru, Kevin Dusling, Dhevan Gangadharan, Jan Fiete Grosse-Oetringhaus, Miklos Gyulassy, Martin Hentschinski, Edmond Iancu, Yuri Kovchegov, Wei Li, Constantin Loizides, Larry McLerran, Peter Petreczky, Bjoern Schenke, Anne Sickles, Derek Teaney, Giorgio Torrieri, Prithwish Tribedy and Konrad Tymoniuk for useful discussions on the topics discussed here. He thanks W. Busza, A. Bzdak, K. Dusling, L. McLerran and B. Schenke for a close reading of the manuscript. NR 75 TC 0 Z9 0 U1 1 U2 2 PU ACADEMIC PRESS INC ELSEVIER SCIENCE PI SAN DIEGO PA 525 B ST, STE 1900, SAN DIEGO, CA 92101-4495 USA SN 0003-4916 EI 1096-035X J9 ANN PHYS-NEW YORK JI Ann. Phys. PD JAN PY 2015 VL 352 SI SI BP 108 EP 116 DI 10.1016/j.aop.2014.08.001 PG 9 WC Physics, Multidisciplinary SC Physics GA CE8VS UT WOS:000352122800013 ER PT S AU Whitelam, S Jack, RL AF Whitelam, Stephen Jack, Robert L. BE Johnson, MA Martinez, TJ TI The Statistical Mechanics of Dynamic Pathways to Self-Assembly SO ANNUAL REVIEW OF PHYSICAL CHEMISTRY, VOL 66 SE Annual Review of Physical Chemistry LA English DT Review; Book Chapter DE phase change; thermodynamics; dynamics ID DENSITY-FUNCTIONAL THEORY; CRYSTAL-NUCLEATION; COMPLEX STRUCTURES; BUILDING-BLOCKS; NONCLASSICAL NUCLEATION; 2-DIMENSIONAL CRYSTALS; HOMOGENEOUS NUCLEATION; COLLOIDAL CRYSTALS; PATCHY PARTICLES; HARD-SPHERES AB This review describes some important physical characteristics of the pathways (i.e., dynamical processes) by which molecular, nanoscale, and micrometer-scale self-assembly occurs. We highlight the existence of features of self-assembly pathways that are common to a wide range of physical systems, even though those systems may differ with respect to their microscopic details. We summarize some existing theoretical descriptions of self-assembly pathways and highlight areas-notably, the description of self-assembly pathways that occur far from equilibrium-that are likely to become increasingly important. C1 [Whitelam, Stephen] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA. [Jack, Robert L.] Univ Bath, Dept Phys, Bath BA2 7AY, Avon, England. RP Whitelam, S (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA. EM swhitelam@lbl.gov; r.jack@bath.ac.uk RI Jack, Robert/M-4096-2014; Foundry, Molecular/G-9968-2014 NR 153 TC 30 Z9 30 U1 11 U2 77 PU ANNUAL REVIEWS PI PALO ALTO PA 4139 EL CAMINO WAY, PO BOX 10139, PALO ALTO, CA 94303-0897 USA SN 0066-426X BN 978-0-8243-1066-0 J9 ANNU REV PHYS CHEM JI Annu. Rev. Phys. Chem. PY 2015 VL 66 BP 143 EP 163 DI 10.1146/annurev-physchem-040214-121215 PG 21 WC Chemistry, Physical SC Chemistry GA BC4BN UT WOS:000352259800007 PM 25493714 ER PT S AU Wang, HF Velarde, L Gan, W Fu, L AF Wang, Hong-Fei Velarde, Luis Gan, Wei Fu, Li BE Johnson, MA Martinez, TJ TI Quantitative Sum-Frequency Generation Vibrational Spectroscopy of Molecular Surfaces and Interfaces: Lineshape, Polarization, and Orientation SO ANNUAL REVIEW OF PHYSICAL CHEMISTRY, VOL 66 SE Annual Review of Physical Chemistry LA English DT Review; Book Chapter DE nonlinear susceptibilities; molecular polarizability; Euler transformation; interference; Fresnel factor; local field factor ID OPTICAL 2ND-HARMONIC GENERATION; AIR-WATER-INTERFACE; CH STRETCHING MODES; LIQUID INTERFACES; NONLINEAR OPTICS; MULTIPOLAR CONTRIBUTIONS; ISOTROPIC FLUIDS; CHIRAL LIQUIDS; SFG-VS; CATALYTIC-REACTIONS AB Sum-frequency generation vibrational spectroscopy (SFG-VS) can provide detailed information and understanding of the molecular composition, interactions, and orientational and conformational structure of surfaces and interfaces through quantitative measurement and analysis. In this review, we present the current status of and discuss important recent developments in the measurement of intrinsic SFG spectral lineshapes and formulations for polarization measurements and orientational analysis of SFG-VS spectra. The focus of this review is to present a coherent description of SFG-VS and discuss the main concepts and issues that can help advance this technique as a quantitative analytical research tool for revealing the chemistry and physics of complex molecular surfaces and interfaces. C1 [Wang, Hong-Fei; Fu, Li] Pacific NW Natl Lab, William R Wiley Environm Mol Sci Lab, Richland, WA 99352 USA. [Velarde, Luis] SUNY Buffalo, Dept Chem, Buffalo, NY 14260 USA. [Gan, Wei] Chinese Acad Sci, Xinjiang Tech Inst Phys & Chem, Urumqi 830011, Xinjiang, Peoples R China. RP Wang, HF (reprint author), Pacific NW Natl Lab, William R Wiley Environm Mol Sci Lab, Richland, WA 99352 USA. EM hongfei.wang@pnnl.gov RI Wang, Hongfei/B-1263-2010; Velarde, Luis/D-4929-2011 OI Wang, Hongfei/0000-0001-8238-1641; Velarde, Luis/0000-0001-6329-3486 NR 148 TC 42 Z9 43 U1 21 U2 95 PU ANNUAL REVIEWS PI PALO ALTO PA 4139 EL CAMINO WAY, PO BOX 10139, PALO ALTO, CA 94303-0897 USA SN 0066-426X BN 978-0-8243-1066-0 J9 ANNU REV PHYS CHEM JI Annu. Rev. Phys. Chem. PY 2015 VL 66 BP 189 EP 216 DI 10.1146/annurev-physchem-040214-121322 PG 28 WC Chemistry, Physical SC Chemistry GA BC4BN UT WOS:000352259800009 PM 25493712 ER PT S AU Zhugayevych, A Tretiak, S AF Zhugayevych, Andriy Tretiak, Sergei BE Johnson, MA Martinez, TJ TI Theoretical Description of Structural and Electronic Properties of Organic Photovoltaic Materials SO ANNUAL REVIEW OF PHYSICAL CHEMISTRY, VOL 66 SE Annual Review of Physical Chemistry LA English DT Review; Book Chapter DE organic solar cell; polarons in organic semiconductors; exciton and charge carrier transport; power conversion efficiency ID HETEROJUNCTION SOLAR-CELLS; 25TH ANNIVERSARY ARTICLE; DENSITY-FUNCTIONAL THEORY; EXCITON DIFFUSION LENGTH; CHARGE-TRANSPORT; CONJUGATED POLYMERS; MOLECULAR-DYNAMICS; AB-INITIO; SEMICONDUCTING POLYMERS; CONDUCTING POLYMERS AB We review recent progress in the modeling of organic solar cells and photovoltaic materials, as well as discuss the underlying theoretical methods with an emphasis on dynamical electronic processes occurring in organic semiconductors. The key feature of the latter is a strong electron-phonon interaction, making the evolution of electronic and structural degrees of freedom inseparable. We discuss commonly used approaches for first-principles modeling of this evolution, focusing on a multiscale framework based on the Holstein-Peierls Hamiltonian solved via polaron transformation. A challenge for both theoretical and experimental investigations of organic solar cells is the complex multiscale morphology of these devices. Nevertheless, predictive modeling of photovoltaic materials and devices is attainable and is rapidly developing, as reviewed here. C1 [Zhugayevych, Andriy; Tretiak, Sergei] Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. [Zhugayevych, Andriy] Skolkovo Inst Sci & Technol, Moscow 143025, Russia. RP Zhugayevych, A (reprint author), Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. EM serg@lanl.gov RI Tretiak, Sergei/B-5556-2009 OI Tretiak, Sergei/0000-0001-5547-3647 NR 215 TC 18 Z9 18 U1 14 U2 107 PU ANNUAL REVIEWS PI PALO ALTO PA 4139 EL CAMINO WAY, PO BOX 10139, PALO ALTO, CA 94303-0897 USA SN 0066-426X BN 978-0-8243-1066-0 J9 ANNU REV PHYS CHEM JI Annu. Rev. Phys. Chem. PY 2015 VL 66 BP 305 EP + DI 10.1146/annurev-physchem-040214-121440 PG 39 WC Chemistry, Physical SC Chemistry GA BC4BN UT WOS:000352259800014 PM 25580623 ER PT J AU Yanez-Serrano, AM Nolscher, AC Williams, J Wolff, S Alves, E Martins, GA Bourtsoukidis, E Brito, J Jardine, K Artaxo, P Kesselmeier, J AF Yanez-Serrano, A. M. Noelscher, A. C. Williams, J. Wolff, S. Alves, E. Martins, G. A. Bourtsoukidis, E. Brito, J. Jardine, K. Artaxo, P. Kesselmeier, J. TI Diel and seasonal changes of biogenic volatile organic compounds within and above an Amazonian rainforest SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID REACTION-MASS-SPECTROMETRY; SOUTHEASTERN UNITED-STATES; METHYL VINYL KETONE; PINUS-SYLVESTRIS L.; PTR-MS MEASUREMENTS; TROPICAL FOREST; COMPOUNDS VOC; ATMOSPHERIC CHEMISTRY; BOUNDARY-LAYER; NONMETHANE HYDROCARBONS AB The Amazonian rainforest is a large tropical ecosystem, which is one of the last pristine continental terrains. This ecosystem is ideally located for the study of diel and seasonal behaviour of biogenic volatile organic compounds (BVOCs) in the absence of local human interference. In this study, we report the first atmospheric BVOC measurements at the Amazonian Tall Tower Observatory (ATTO) site, located in central Amazonia. A quadrupole proton-transfer-reaction mass spectrometer (PTR-MS), with seven ambient air inlets, positioned from near ground to about 80 m (0.05, 0.5, 4, 24, 38, 53 and 79 m above the forest floor), was deployed for BVOC monitoring. We report diel and seasonal (February-March 2013 as wet season and September 2013 as dry season) ambient mixing ratios for isoprene, monoterpenes, isoprene oxidation products, acetaldehyde, acetone, methyl ethyl ketone (MEK), methanol and acetonitrile. Clear diel and seasonal patterns were observed for all compounds. In general, lower mixing ratios were observed during night, while maximum mixing ratios were observed during the wet season (February-March 2013), with the peak in solar irradiation at 12:00 LT (local time) and during the dry season (September 2013) with the peak in temperature at 16:00 LT. Isoprene and monoterpene mixing ratios were the highest within the canopy with a median of 7.6 and 1 ppb, respectively (interquartile range (IQR) of 6.1 and 0.38 ppb) during the dry season (at 24 m, from 12:00 to 15:00 LT). The increased contribution of oxygenated volatile organic compounds (OVOCs) above the canopy indicated a transition from dominating forest emissions during the wet season (when mixing ratios were higher than within the canopy), to a blend of biogenic emission, photochemical production and advection during the dry season when mixing ratios were higher above the canopy. Our observations suggest strong seasonal interactions between environmental (insolation, temperature) and biological (phenology) drivers of leaf BVOC emissions and atmospheric chemistry. Considerable differences in the magnitude of BVOC mixing ratios, as compared to other reports of Amazonian BVOC, demonstrate the need for long-term observations at different sites and more standardized measurement procedures, in order to better characterize the natural exchange of BVOCs between the Amazonian rainforest and the atmosphere. C1 [Yanez-Serrano, A. M.; Wolff, S.; Kesselmeier, J.] Max Planck Inst Chem, Biogeochem Dept, D-55020 Mainz, Germany. [Noelscher, A. C.; Williams, J.; Bourtsoukidis, E.] Max Planck Inst Chem, Atmospher Chem Dept, D-55020 Mainz, Germany. [Yanez-Serrano, A. M.; Wolff, S.; Alves, E.; Martins, G. A.; Jardine, K.] INPA, BR-69083000 Manaus, Amazonas, Brazil. [Brito, J.; Artaxo, P.] Univ Fed Sao Paulo, Inst Fis, BR-05508900 Sao Paulo, SP, Brazil. [Jardine, K.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. RP Yanez-Serrano, AM (reprint author), Max Planck Inst Chem, Biogeochem Dept, POB 3060, D-55020 Mainz, Germany. EM ayanezserrano@mpic.de RI Brito, Joel/B-6181-2013; Kesselmeier, Jurgen/E-2389-2016; Artaxo, Paulo/E-8874-2010; Jardine, Kolby/N-2802-2013; OI Brito, Joel/0000-0002-4420-9442; Kesselmeier, Jurgen/0000-0002-4446-534X; Artaxo, Paulo/0000-0001-7754-3036; Jardine, Kolby/0000-0001-8491-9310; YANEZ SERRANO, ANA MARIA/0000-0001-6408-5961 FU Max Planck Society; Instituto Nacional de Pesquisas da Amazonia; ATTO project (German Federal Ministry of Education and Research); ATTO project (BMBF) [01LB1001A]; ATTO project (Brazilian Ministerio da Ciencia, Tecnologia e Inovacao FINEP/MCTI) [01.11.01248.00]; UEA; FAPEAM; LBA/INPA; SDS/CEUC/RDS-Uatuma FX We thank the Max Planck Society and the Instituto Nacional de Pesquisas da Amazonia for continuous support. Furthermore, we acknowledge the support by the ATTO project (German Federal Ministry of Education and Research, BMBF funds 01LB1001A; Brazilian Ministerio da Ciencia, Tecnologia e Inovacao FINEP/MCTI contract 01.11.01248.00); UEA and FAPEAM, LBA/INPA and SDS/CEUC/RDS-Uatuma. We would like to especially thank all the people involved in the logistical support of the ATTO project, in particular Reiner Ditz and Hermes Braga Xavier. We acknowledge the Micrometeorological group of the INPA/LBA for their collaboration concerning the meteorological parameters, with special thanks to Marta Sa, Antonio Huxley and Leonardo Oliveira. We are grateful to Tracey W. Andreae for help with the manuscript, Guenther Schebeske for the GC-FID analysis and Nina Knothe for logistical help. We would also like to thank Thomas Klupfel for all the great support provided with the PTR-MS operation in the laboratory as well as in the field. Lastly, we would like to acknowledge the referees of this manuscript for the extensive contributions and suggestions which helped to improve this study. NR 114 TC 9 Z9 9 U1 6 U2 42 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1680-7316 EI 1680-7324 J9 ATMOS CHEM PHYS JI Atmos. Chem. Phys. PY 2015 VL 15 IS 6 BP 3359 EP 3378 DI 10.5194/acp-15-3359-2015 PG 20 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA CE9IN UT WOS:000352157600024 ER PT J AU Boda, D Leaf, G Fonseca, J Eisenberg, B AF Boda, D. Leaf, G. Fonseca, J. Eisenberg, B. TI Energetics of ion competition in the DEKA selectivity filter of neuronal sodium channels SO CONDENSED MATTER PHYSICS LA English DT Article DE Monte Carlo; primitive model electrolytes; ion channel; selectivity ID MONTE-CARLO SIMULATIONS; EPITHELIAL NA+ CHANNEL; MODEL CALCIUM-CHANNEL; PERFUSED GIANT AXONS; BROWNIAN DYNAMICS; MYELINATED NERVE; ORGANIC CATIONS; FROG-MUSCLE; SIDE-CHAINS; PORE AB The energetics of ionic selectivity in the neuronal sodium channels is studied. A simple model constructed for the selectivity filter of the channel is used. The selectivity filter of this channel type contains aspartate (D), glutamate (E), lysine (K), and alanine (A) residues (the DEKA locus). We use Grand Canonical Monte Carlo simulations to compute equilibrium binding selectivity in the selectivity filter and to obtain various terms of the excess chemical potential from a particle insertion procedure based on Widom's method. We show that K+ ions in competition with Na+ are efficiently excluded from the selectivity filter due to entropic hard sphere exclusion. The dielectric constant of protein has no effect on this selectivity. Ca2+ ions, on the other hand, are excluded from the filter due to a free energetic penalty which is enhanced by the low dielectric constant of protein. C1 [Boda, D.] Univ Pannonia, Dept Phys Chem, H-8201 Veszprem, Hungary. [Leaf, G.] Argonne Natl Lab, Math & Comp Sci Div, Argonne, IL 60439 USA. [Fonseca, J.] Purdue Univ, Network Computat Nanotechnol, W Lafayette, IN 47907 USA. [Eisenberg, B.] Rush Univ, Med Ctr, Dept Mol Biophys & Physiol, Chicago, IL 60612 USA. RP Boda, D (reprint author), Univ Pannonia, Dept Phys Chem, POB 158, H-8201 Veszprem, Hungary. EM boda@almos.vein.hu FU Hungarian National Research Fund in the framework of ERA Chemistry [OTKA NN113527]; [TAMOP-4.2.2/A-11/1/KONV-2012-0071]; [TAMOP-4.1.1/C-12/1/KONV-2012-0017] FX We gratefully acknowledge the computing resources provided on Blues and/or Fusion, high-performance computing cluster operated by the Laboratory Computing Resource Center at Argonne National Laboratory. We acknowledge the support of the Hungarian National Research Fund (OTKA NN113527) in the framework of ERA Chemistry. Present publication was realized with the support of the projects TAMOP-4.2.2/A-11/1/KONV-2012-0071 and TAMOP-4.1.1/C-12/1/KONV-2012-0017. NR 75 TC 2 Z9 2 U1 0 U2 10 PU INST CONDENSED MATTER PHYSICS NATL ACAD SCIENCES UKRAINE PI LVIV PA 1 SVIENTSITSKII STR, LVIV, 79011, UKRAINE SN 1607-324X EI 2224-9079 J9 CONDENS MATTER PHYS JI Condens. Matter Phys. PY 2015 VL 18 IS 1 AR 13601 DI 10.5488/CMP.18.13601 PG 14 WC Physics, Condensed Matter SC Physics GA CF6NI UT WOS:000352673000008 ER PT J AU Mamun, MA Baumgart, H Elmustafa, AA AF Mamun, M. A. Baumgart, H. Elmustafa, A. A. TI ALD Zirconium Oxide (ZrO2) Thin Films Mechanical/Structural Properties for High-Tech Applications SO ECS JOURNAL OF SOLID STATE SCIENCE AND TECHNOLOGY LA English DT Article ID CRYSTALLINE SILICON; DEPOSITION; SUBSTRATE AB The nanomechanical and structural properties of atomic layer deposition (ALD) zirconium oxide (ZrO2) films of varying thickness deposited on p-type Si (100) substrates with 200, 300, and 500, ALD deposition cycles were investigated. The 300 ALD deposition cycles ZrO2 films were further annealed at 600 degrees C. The nanomechanical properties of the films were tested using nanoindentation and the surface morphology was investigated using AFM. The structural and surface properties were explored using field emission scanning electron microscopy (FE-SEM) and atomic force microscopy (AFM). We discuss the influence of the deposition technique on the structure and properties of the ZrO2 films resulting from ALD synthesis. The nanoindentation results indicate that the films become consistently softer as the number of ALD deposition cycles increase and the film grows thicker. Further annealing of the films at 600 degrees C slightly enhanced the hardness and fracture toughness of the films. The annealed ALD films depicted shorter radial cracks compared to the films under the same applied stress, which were not annealed in forming gas. (C) 2015 The Electrochemical Society. All rights reserved. C1 [Mamun, M. A.; Elmustafa, A. A.] Old Dominion Univ, Dept Mech & Aerosp Engn, Norfolk, VA 23529 USA. [Mamun, M. A.; Baumgart, H.; Elmustafa, A. A.] Appl Res Ctr, Thomas Jefferson Lab, Newport News, VA 23606 USA. [Baumgart, H.] Old Dominion Univ, Dept Elect & Comp Engn, Norfolk, VA 23529 USA. RP Mamun, MA (reprint author), Old Dominion Univ, Dept Mech & Aerosp Engn, Norfolk, VA 23529 USA. EM aelmusta@odu.edu NR 14 TC 1 Z9 1 U1 1 U2 16 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 2162-8769 J9 ECS J SOLID STATE SC JI ECS J. Solid State Sci. Technol. PY 2015 VL 4 IS 5 BP Q35 EP Q37 DI 10.1149/2.0051505jss PG 3 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA CF0HP UT WOS:000352224200021 ER PT J AU Bailie, CD Christoforo, MG Mailoa, JP Bowring, AR Unger, EL Nguyen, WH Burschka, J Pellet, N Lee, JZ Gratzel, M Noufi, R Buonassisi, T Salleo, A McGehee, MD AF Bailie, Colin D. Christoforo, M. Greyson Mailoa, Jonathan P. Bowring, Andrea R. Unger, Eva L. Nguyen, William H. Burschka, Julian Pellet, Norman Lee, Jungwoo Z. Graetzel, Michael Noufi, Rommel Buonassisi, Tonio Salleo, Alberto McGehee, Michael D. TI Semi-transparent perovskite solar cells for tandems with silicon and CIGS SO ENERGY & ENVIRONMENTAL SCIENCE LA English DT Article ID ORGANOMETAL HALIDE PEROVSKITES; EFFICIENCY; DEPOSITION; PHOTOVOLTAICS; TRANSMISSION; PERFORMANCE; ELECTRODES AB A promising approach for upgrading the performance of an established low-bandgap solar technology without adding much cost is to deposit a high bandgap polycrystalline semiconductor on top to make a tandem solar cell. We use a transparent silver nanowire electrode on perovskite solar cells to achieve a semi-transparent device. We place the semi-transparent cell in a mechanically-stacked tandem configuration onto copper indium gallium diselenide (CIGS) and low-quality multicrystalline silicon (Si) to achieve solid-state polycrystalline tandem solar cells with a net improvement in efficiency over the bottom cell alone. This work paves the way for integrating perovskites into a low-cost and high-efficiency (>25%) tandem cell. C1 [Bailie, Colin D.; Bowring, Andrea R.; Unger, Eva L.; Salleo, Alberto; McGehee, Michael D.] Stanford Univ, Dept Mat Sci & Engn, Stanford, CA 94305 USA. [Christoforo, M. Greyson] Stanford Univ, Dept Elect Engn, Stanford, CA 94305 USA. [Mailoa, Jonathan P.; Lee, Jungwoo Z.; Buonassisi, Tonio] MIT, Sch Engn, Cambridge, MA 02139 USA. [Nguyen, William H.] Stanford Univ, Dept Chem, Stanford, CA 94305 USA. [Burschka, Julian; Pellet, Norman; Graetzel, Michael] Ecole Polytech Fed Lausanne, Inst Sci & Ingn Chim, Lab Photon & Interfaces, CH-1015 Lausanne, Switzerland. [Noufi, Rommel] Natl Renewable Energy Lab, Golden, CO 80401 USA. RP Bailie, CD (reprint author), Stanford Univ, Dept Mat Sci & Engn, Stanford, CA 94305 USA. EM mmcgehee@stanford.edu RI Bailie, Colin/K-8142-2013 OI Bailie, Colin/0000-0001-9203-2656 FU Department of Energy [DE-EE0004946]; Center for Advanced Molecular Photovoltaics by the King Abdullah University of Science and Technology (KAUST) [KUS-C1-015-21]; Global Climate and Energy Project (GCEP); National Science Foundation [ARI-0963061, ECS-0335765]; National Research Foundation Singapore through the Singapore MIT Alliance for Research and Technology's Low Energy Electronic Systems research program; Department of Defense (DoD) through the National Defense Science & Engineering Graduate Fellowship (NDSEG) Program FX This work was primarily supported by the Department of Energy through the Bay Area Photovoltaic Consortium under Award Number DE-EE0004946. This material was also based on work supported by the Center for Advanced Molecular Photovoltaics under Award Number KUS-C1-015-21 by the King Abdullah University of Science and Technology (KAUST), and the Global Climate and Energy Project (GCEP). The nanowire electrode fabrication work was performed in part at the Stanford Nano-fabrication Facility's nSiL lab, which was funded by National Science Foundation award ARI-0963061. The muticrystalline silicon device fabrication was performed in part at the Harvard Center for Nanoscale Systems, which was funded by National Science Foundation award ECS-0335765. Jonathan P. Mailoa and Jungwoo Z. Lee were supported by the National Research Foundation Singapore through the Singapore MIT Alliance for Research and Technology's Low Energy Electronic Systems research program. A.E. Morishige and J. Hofstetter (MIT) are acknowledged for supplying and advice on preparing the silicon wafers. William H. Nguyen was supported by the Department of Defense (DoD) through the National Defense Science & Engineering Graduate Fellowship (NDSEG) Program. We thank Dmitry Poplavskyy and DuPont for their generous donation of mono-crystalline silicon solar cells. We acknowledge helpful feedback from an anonymous reviewer. NR 37 TC 142 Z9 144 U1 67 U2 353 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1754-5692 EI 1754-5706 J9 ENERG ENVIRON SCI JI Energy Environ. Sci. PY 2015 VL 8 IS 3 BP 956 EP 963 DI 10.1039/c4ee03322a PG 8 WC Chemistry, Multidisciplinary; Energy & Fuels; Engineering, Chemical; Environmental Sciences SC Chemistry; Energy & Fuels; Engineering; Environmental Sciences & Ecology GA CF0ZZ UT WOS:000352274600021 ER PT J AU Liu, M Rong, ZQ Malik, R Canepa, P Jain, A Ceder, G Persson, KA AF Liu, Miao Rong, Ziqin Malik, Rahul Canepa, Pieremanuele Jain, Anubhav Ceder, Gerbrand Persson, Kristin A. TI Spinel compounds as multivalent battery cathodes: a systematic evaluation based on ab initio calculations SO ENERGY & ENVIRONMENTAL SCIENCE LA English DT Article ID GENERALIZED GRADIENT APPROXIMATION; RECHARGEABLE MAGNESIUM BATTERIES; SECONDARY LITHIUM BATTERIES; 1ST PRINCIPLES CALCULATIONS; POLYVALENT CATIONS; ENERGY-STORAGE; ION BATTERIES; MG BATTERIES; METAL-OXIDES; INTERCALATION AB Batteries that shuttle multivalent ions such as Mg2+ and Ca2+ ions are promising candidates for achieving higher energy density than available with current Li-ion technology. Finding electrode materials that reversibly store and release these multivalent cations is considered a major challenge for enabling such multivalent battery technology. In this paper, we use recent advances in high-throughput first-principles calculations to systematically evaluate the performance of compounds with the spinel structure as multivalent intercalation cathode materials, spanning a matrix of five different intercalating ions and seven transition metal redox active cations. We estimate the insertion voltage, capacity, thermodynamic stability of charged and discharged states, as well as the intercalating ion mobility and use these properties to evaluate promising directions. Our calculations indicate that the Mn2O4 spinel phase based on Mg and Ca are feasible cathode materials. In general, we find that multivalent cathodes exhibit lower voltages compared to Li cathodes; the voltages of Ca spinels are similar to 0.2 V higher than those of Mg compounds (versus their corresponding metals), and the voltages of Mg compounds are similar to 1.4 V higher than Zn compounds; consequently, Ca and Mg spinels exhibit the highest energy densities amongst all the multivalent cation species. The activation barrier for the Al3+ ion migration in the Mn2O4 spinel is very high (similar to 1400 meV for Al3+ in the dilute limit); thus, the use of an Al based Mn spinel intercalation cathode is unlikely. Amongst the choice of transition metals, Mn-based spinel structures rank highest when balancing all the considered properties. C1 [Liu, Miao; Jain, Anubhav; Persson, Kristin A.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. [Rong, Ziqin; Malik, Rahul; Canepa, Pieremanuele; Ceder, Gerbrand] MIT, Dept Mat Sci & Engn, Cambridge, MA 02139 USA. RP Liu, M (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. EM kapersson@lbl.gov RI Canepa, Pieremanuele/O-2344-2013; Liu, Miao/N-9937-2013 OI Canepa, Pieremanuele/0000-0002-5168-9253; Liu, Miao/0000-0002-1843-9519 FU Joint Center for Energy Storage Research (JCESR), an Energy Innovation Hub - U.S. Department of Energy, Office of Science, Basic Energy Sciences; Assistant Secretary for Energy Efficiency and Renewable Energy [DEAC02-05CH11231]; BES DOE Grant [EDCBEE] FX This work was intellectually led and fully supported by of the Joint Center for Energy Storage Research (JCESR), an Energy Innovation Hub funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences. Work at the Lawrence Berkeley National Laboratory was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, under Contract no. DEAC02-05CH11231. We also thank the National Energy Research Scientific Computing Center (NERSC) for providing computing resources. The Materials Project (BES DOE Grant no. EDCBEE) is acknowledged for infrastructure and algorithmic support. NR 69 TC 47 Z9 47 U1 37 U2 174 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1754-5692 EI 1754-5706 J9 ENERG ENVIRON SCI JI Energy Environ. Sci. PY 2015 VL 8 IS 3 BP 964 EP 974 DI 10.1039/c4ee03389b PG 11 WC Chemistry, Multidisciplinary; Energy & Fuels; Engineering, Chemical; Environmental Sciences SC Chemistry; Energy & Fuels; Engineering; Environmental Sciences & Ecology GA CF0ZZ UT WOS:000352274600022 ER PT J AU Yan, J Gorai, P Ortiz, B Miller, S Barnett, SA Mason, T Stevanovic, V Toberer, ES AF Yan, Jun Gorai, Prashun Ortiz, Brenden Miller, Sam Barnett, Scott A. Mason, Thomas Stevanovic, Vladan Toberer, Eric S. TI Material descriptors for predicting thermoelectric performance SO ENERGY & ENVIRONMENTAL SCIENCE LA English DT Article ID METAL-INSULATOR-TRANSITION; THERMAL-CONDUCTIVITY; TRANSPORT-PROPERTIES; ENERGY-CONVERSION; ZINTL COMPOUND; EFFICIENCY; BAND; CRYSTALS; OXIDE; PBTE AB In the context of materials design and high-throughput computational searches for new thermoelectric materials, the need to compute electron and phonon transport properties renders direct assessment of the thermoelectric figure of merit (zT) for large numbers of compounds untenable. Here we develop a semi-empirical approach rooted in first-principles calculations that allows relatively simple computational assessment of the intrinsic bulk material properties which govern zT. These include carrier mobility, effective mass, and lattice thermal conductivity, which combine to form a semi-empirical metric (descriptor) termed beta(SE). We assess the predictive power of beta(SE) against a range of known thermoelectric materials, as well as demonstrate its use in high-throughput screening for promising candidate materials. C1 [Yan, Jun; Gorai, Prashun; Ortiz, Brenden; Stevanovic, Vladan; Toberer, Eric S.] Colorado Sch Mines, Golden, CO 80401 USA. [Gorai, Prashun; Stevanovic, Vladan; Toberer, Eric S.] Natl Renewable Energy Lab, Golden, CO USA. [Miller, Sam; Barnett, Scott A.; Mason, Thomas] Northwestern Univ, Evanston, IL USA. RP Yan, J (reprint author), Colorado Sch Mines, Golden, CO 80401 USA. EM etoberer@mines.edu RI Barnett, Scott/B-7502-2009; Mason, Thomas/B-7528-2009 FU NSF DMR program [1334713, 1333335] FX We acknowledge support from the NSF DMR program, grant no. 1334713 and 1333335. The use of NREL's computing resources is gratefully acknowledged. NR 102 TC 37 Z9 37 U1 20 U2 93 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1754-5692 EI 1754-5706 J9 ENERG ENVIRON SCI JI Energy Environ. Sci. PY 2015 VL 8 IS 3 BP 983 EP 994 DI 10.1039/c4ee03157a PG 12 WC Chemistry, Multidisciplinary; Energy & Fuels; Engineering, Chemical; Environmental Sciences SC Chemistry; Energy & Fuels; Engineering; Environmental Sciences & Ecology GA CF0ZZ UT WOS:000352274600024 ER PT J AU Wang, HL Turner, JA AF Wang, Heli Turner, John A. TI Photoelectrochemical reduction of nitrates at the illuminated p-GaInP2 photoelectrode (vol 6, pg 1802, 2013) SO ENERGY & ENVIRONMENTAL SCIENCE LA English DT Correction C1 [Wang, Heli; Turner, John A.] Natl Renewable Energy Lab, Golden, CO 80401 USA. RP Wang, HL (reprint author), Natl Renewable Energy Lab, 15013 Denver West Pkwy, Golden, CO 80401 USA. EM heli.wang@nrel.gov NR 1 TC 0 Z9 0 U1 4 U2 21 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1754-5692 EI 1754-5706 J9 ENERG ENVIRON SCI JI Energy Environ. Sci. PY 2015 VL 8 IS 3 BP 1046 EP 1046 DI 10.1039/c5ee90006a PG 1 WC Chemistry, Multidisciplinary; Energy & Fuels; Engineering, Chemical; Environmental Sciences SC Chemistry; Energy & Fuels; Engineering; Environmental Sciences & Ecology GA CF0ZZ UT WOS:000352274600031 ER PT J AU Wang, JJ Sun, XL AF Wang, Jiajun Sun, Xueliang TI Olivine LiFePO4: the remaining challenges for future energy storage SO ENERGY & ENVIRONMENTAL SCIENCE LA English DT Review ID LITHIUM-ION BATTERIES; HIGH-PERFORMANCE CATHODE; ENHANCED ELECTROCHEMICAL PERFORMANCE; HYDROTHERMALLY SYNTHESIZED LIFEPO4; POLYMERIZATION RESTRICTION METHOD; SOLID-SOLUTION PHASES; MELT CASTING LIFEPO4; X-RAY MICROSCOPY; LI-ION; SODIUM-ION AB Rechargeable batteries can effectively store electrical energy as chemical energy, and release it when needed, providing a good choice for applications in electric vehicles (EVs). Naturally, safety concerns are the key issue for the application of battery technology in EVs. Olivine LiFePO4 is considered to be the most promising cathode material for lithium-ion batteries due to its environmental friendliness, high cycling performance and safety characteristics. Some important breakthroughs in recent years have allowed its successful commercialization. However, in spite of its success, the commercial application of LiFePO4 batteries in EVs is still hindered by some technological obstacles. Herein, we provide an update on our previous review, and overview the most significant advances in the remaining challenges for this promising battery material. New research directions and future trends have also been discussed. C1 [Wang, Jiajun; Sun, Xueliang] Univ Western Ontario, Dept Mech & Mat Engn, London, ON N6A 5B9, Canada. RP Wang, JJ (reprint author), Brookhaven Natl Lab, Natl Synchrotron Light Source 2, Upton, NY 11973 USA. EM xsun@eng.uwo.ca RI Sun, Xueliang/C-7257-2012; wang, jiajun/H-3315-2012; wang, jiajun/H-5683-2016 FU Nature Sciences and Engineering Research Council of Canada (NSERC); Canada Research Chair (CRC) Program; Canada Foundation for Innovation (CFI); Ontario Research Fund (ORF); Canada Light Source (CLS) at University of Saskatchewan; Canadian Centre for Electron Microscopy (CCEM) at McMaster University; University of Western Ontario FX This work was supported by Nature Sciences and Engineering Research Council of Canada (NSERC), Canada Research Chair (CRC) Program, Canada Foundation for Innovation (CFI), Ontario Research Fund (ORF), the Canada Light Source (CLS) at University of Saskatchewan, the Canadian Centre for Electron Microscopy (CCEM) at McMaster University, and University of Western Ontario. We gratefully acknowledge Craig Langford and Kaixi Wang for their help in the discussion and English polishing for this paper. NR 249 TC 62 Z9 62 U1 61 U2 336 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1754-5692 EI 1754-5706 J9 ENERG ENVIRON SCI JI Energy Environ. Sci. PY 2015 VL 8 IS 4 BP 1110 EP 1138 DI 10.1039/c4ee04016c PG 29 WC Chemistry, Multidisciplinary; Energy & Fuels; Engineering, Chemical; Environmental Sciences SC Chemistry; Energy & Fuels; Engineering; Environmental Sciences & Ecology GA CF1AI UT WOS:000352275500003 ER PT J AU Simon, CM Kim, J Gomez-Gualdron, DA Camp, JS Chung, YG Martin, RL Mercado, R Deem, MW Gunter, D Haranczyk, M Sholl, DS Snurr, RQ Smit, B AF Simon, Cory M. Kim, Jihan Gomez-Gualdron, Diego A. Camp, Jeffrey S. Chung, Yongchul G. Martin, Richard L. Mercado, Rocio Deem, Michael W. Gunter, Dan Haranczyk, Maciej Sholl, David S. Snurr, Randall Q. Smit, Berend TI The materials genome in action: identifying the performance limits for methane storage SO ENERGY & ENVIRONMENTAL SCIENCE LA English DT Article ID METAL-ORGANIC FRAMEWORKS; NATURAL-GAS STORAGE; NANOPOROUS MATERIALS; POROUS MATERIALS; BUILDING UNITS; CARBON-CAPTURE; FORCE-FIELD; SIMULATIONS; SEPARATIONS; CHALLENGES AB Analogous to the way the Human Genome Project advanced an array of biological sciences by mapping the human genome, the Materials Genome Initiative aims to enhance our understanding of the fundamentals of materials science by providing the information we need to accelerate the development of new materials. This approach is particularly applicable to recently developed classes of nanoporous materials, such as metal-organic frameworks (MOFs), which are synthesized from a limited set of molecular building blocks that can be combined to generate a very large number of different structures. In this Perspective, we illustrate how a materials genome approach can be used to search for high-performance adsorbent materials to store natural gas in a vehicular fuel tank. Drawing upon recent reports of large databases of existing and predicted nanoporous materials generated in silico, we have collected and compared on a consistent basis the methane uptake in over 650 000 materials based on the results of molecular simulation. The data that we have collected provide candidate structures for synthesis, reveal relationships between structural characteristics and performance, and suggest that it may be difficult to reach the current Advanced Research Project Agency-Energy (ARPA-E) target for natural gas storage. C1 [Simon, Cory M.; Smit, Berend] Univ Calif Berkeley, Dept Chem & Biomol Engn, Berkeley, CA 94720 USA. [Kim, Jihan] Korea Adv Inst Sci & Technol, Dept Chem & Biomol Engn, Taejon 305701, South Korea. [Gomez-Gualdron, Diego A.; Chung, Yongchul G.; Snurr, Randall Q.] Northwestern Univ, Dept Chem & Biol Engn, Evanston, IL 60208 USA. [Camp, Jeffrey S.; Sholl, David S.] Georgia Inst Technol, Sch Chem & Biomol Engn, Atlanta, GA 30332 USA. [Martin, Richard L.; Gunter, Dan; Haranczyk, Maciej] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Computat Res Div, Berkeley, CA 94720 USA. [Mercado, Rocio; Smit, Berend] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Deem, Michael W.] Rice Univ, Dept Bioengn, Houston, TX 77005 USA. [Deem, Michael W.] Rice Univ, Dept Phys & Astron, Houston, TX 77005 USA. [Smit, Berend] EPFL, Inst Sci & Ingn Chim Valais, Lab Mol Simulat, CH-1950 Sion, Switzerland. [Martin, Richard L.] IBM Almaden Res Ctr, Watson Grp, San Jose, CA 95120 USA. RP Snurr, RQ (reprint author), Northwestern Univ, Dept Chem & Biol Engn, Evanston, IL 60208 USA. EM snurr@northwestern.edu; Berend-Smit@berkeley.edu RI Smit, Berend/B-7580-2009; Snurr, Randall/B-6699-2009; Chung, Yongchul/G-7017-2015; Haranczyk, Maciej/A-6380-2014; Kim, Jihan/H-8002-2013; Deem, Michael/P-3595-2014; OI Smit, Berend/0000-0003-4653-8562; Chung, Yongchul/0000-0002-7756-0589; Haranczyk, Maciej/0000-0001-7146-9568; Deem, Michael/0000-0002-4298-3450; Simon, Cory/0000-0002-8181-9178 FU U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences [DE-FG02-12ER16362] FX The research was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences under Award DE-FG02-12ER16362. NR 57 TC 49 Z9 50 U1 21 U2 103 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1754-5692 EI 1754-5706 J9 ENERG ENVIRON SCI JI Energy Environ. Sci. PY 2015 VL 8 IS 4 BP 1190 EP 1199 DI 10.1039/c4ee03515a PG 10 WC Chemistry, Multidisciplinary; Energy & Fuels; Engineering, Chemical; Environmental Sciences SC Chemistry; Energy & Fuels; Engineering; Environmental Sciences & Ecology GA CF1AI UT WOS:000352275500006 ER PT J AU Guo, SH Yu, HJ Liu, P Ren, Y Zhang, T Chen, MW Ishida, M Zhou, HS AF Guo, Shaohua Yu, Haijun Liu, Pan Ren, Yang Zhang, Tao Chen, Mingwei Ishida, Masayoshi Zhou, Haoshen TI High-performance symmetric sodium-ion batteries using a new, bipolar O3-type material, Na0.8Ni0.4Ti0.6O2 SO ENERGY & ENVIRONMENTAL SCIENCE LA English DT Article ID ENERGY-STORAGE; ELECTROCHEMICAL PROPERTIES; LONG-LIFE; REVERSIBLE ELECTRODE; POSITIVE ELECTRODE; LITHIUM BATTERIES; SOLID-ELECTROLYTE; CATHODE MATERIALS; CYCLE LIFE; NA AB Based on low-cost and rich resources, sodium-ion batteries have been regarded as a promising candidate for next-generation energy storage batteries in the large-scale energy applications of renewable energy and smart grids. However, there are some critical drawbacks limiting its application, such as safety and stability problems. In this work, a stable symmetric sodium-ion battery based on the bipolar, active O3-type material, Na0.8Ni0.4Ti0.6O2, is developed. This bipolar material shows a typical O3-type layered structure, containing two electrochemically active transition metals with redox couples of Ni4+/Ni2+ and Ti4+/Ti3+, respectively. This Na0.8Ni0.4Ti0.6O2-based symmetric cell exhibits a high average voltage of 2.8 V, a reversible discharge capacity of 85 mA h g(-1), 75% capacity retention after 150 cycles and good rate capability. This full symmetric cell will greatly contribute to the development of room-temperature sodium-ion batteries with a view towards safety, low cost and long life, and it will stimulate further research on symmetric cells using the same active materials as both cathode and anode. C1 [Guo, Shaohua; Yu, Haijun; Zhang, Tao; Zhou, Haoshen] Natl Inst Adv Ind Sci & Technol, Energy Technol Res Inst, Tsukuba, Ibaraki, Japan. [Guo, Shaohua; Ishida, Masayoshi; Zhou, Haoshen] Univ Tsukuba, Grad Sch Syst & Informat Engn, Tsukuba, Ibaraki 3058573, Japan. [Liu, Pan; Chen, Mingwei] Tohoku Univ, WPI Adv Inst Mat Res, Sendai, Miyagi 9808577, Japan. [Ren, Yang] Argonne Natl Lab, Argonne, IL 60439 USA. [Zhou, Haoshen] Nanjing Univ, Natl Lab Solid State Microstruct, Nanjing 210093, Jiangsu, Peoples R China. [Zhou, Haoshen] Nanjing Univ, Dept Energy Sci & Engn, Nanjing 210093, Jiangsu, Peoples R China. RP Yu, HJ (reprint author), Natl Inst Adv Ind Sci & Technol, Energy Technol Res Inst, Tsukuba, Ibaraki, Japan. EM haijun-yu@aist.go.jp; hs.zhou@aist.go.jp RI Chen, Mingwei/A-4855-2010; Liu, Pan/H-5469-2012; Yu, Haijun/J-4981-2014; 郭, 少华/R-8504-2016 OI Chen, Mingwei/0000-0002-2850-8872; Liu, Pan/0000-0002-4063-9605; Yu, Haijun/0000-0003-0204-9943; 郭, 少华/0000-0003-0818-8354 FU CSC (China Scholarship Council); World-leading Innovative R&D on Science and Technology; U. S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357] FX S. H. Guo is grateful for the financial support of the CSC (China Scholarship Council) scholarship. This work was supported by the Innovative Basic Research toward Creation of High-performance Battery in Funding Program for World-leading Innovative R&D on Science and Technology. Use of the Advanced Photon Source at Argonne National Laboratory was supported by the U. S. Department of Energy, Office of Science, Office of Basic Energy Sciences, (DE-AC02-06CH11357). NR 61 TC 41 Z9 41 U1 28 U2 118 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1754-5692 EI 1754-5706 J9 ENERG ENVIRON SCI JI Energy Environ. Sci. PY 2015 VL 8 IS 4 BP 1237 EP 1244 DI 10.1039/c4ee03361b PG 8 WC Chemistry, Multidisciplinary; Energy & Fuels; Engineering, Chemical; Environmental Sciences SC Chemistry; Energy & Fuels; Engineering; Environmental Sciences & Ecology GA CF1AI UT WOS:000352275500011 ER PT J AU Fang, Y Liu, C Leung, LR AF Fang, Y. Liu, C. Leung, L. R. TI Accelerating the spin-up of the coupled carbon and nitrogen cycle model in CLM4 SO GEOSCIENTIFIC MODEL DEVELOPMENT LA English DT Article ID LEAF-AREA INDEX; STEADY-STATE; LAND MODEL; SOIL BIOGEOCHEMISTRY; USE EFFICIENCY; ENERGY FLUXES; WATER-VAPOR; ECOSYSTEM; FOREST; DIOXIDE AB The commonly adopted biogeochemistry spin-up process in an Earth system model (ESM) is to run the model for hundreds to thousands of years subject to periodic atmospheric forcing to reach dynamic steady state of the carbon-nitrogen (CN) models. A variety of approaches have been proposed to reduce the computation time of the spin-up process. Significant improvement in computational efficiency has been made recently. However, a long simulation time is still required to reach the common convergence criteria of the coupled carbon-nitrogen model. A gradient projection method was proposed and used to further reduce the computation time after examining the trend of the dominant carbon pools. The Community Land Model version 4 (CLM4) with a carbon and nitrogen component was used in this study. From point-scale simulations, we found that the method can reduce the computation time by 20-69% compared to one of the fastest approaches in the literature. We also found that the cyclic stability of total carbon for some cases differs from that of the periodic atmospheric forcing, and some cases even showed instability. Close examination showed that one case has a carbon periodicity much longer than that of the atmospheric forcing due to the annual fire disturbance that is longer than half a year. The rest was caused by the instability of water table calculation in the hydrology model of CLM4. The instability issue is resolved after we replaced the hydrology scheme in CLM4 with a flow model for variably saturated porous media. C1 [Fang, Y.] Pacific NW Natl Lab, Hydrol Grp, Energy & Environm Directorate, Richland, WA 99352 USA. [Liu, C.] Pacific NW Natl Lab, Geochem Grp, Fundamental & Computat Sci Directorate, Richland, WA 99352 USA. [Leung, L. R.] Pacific NW Natl Lab, Atmospher Sci & Global Change Div, Fundamental & Computat Sci Directorate, Richland, WA 99352 USA. RP Fang, Y (reprint author), Pacific NW Natl Lab, Hydrol Grp, Energy & Environm Directorate, Richland, WA 99352 USA. EM yilin.fang@pnnl.gov RI Liu, Chongxuan/C-5580-2009; Fang, Yilin/J-5137-2015 FU Pacific Northwest National Laboratory's Laboratory Directed Research and Development Program; US Department of Energy [DE-AC05-76RL01830] FX This research has been accomplished through funding support from Pacific Northwest National Laboratory's Laboratory Directed Research and Development Program. We thank the North American Carbon Program Site-Level Interim Synthesis team, the Large Scale Biosphere-Atmosphere Experiment in Amazonia Model Intercomparison Project team, and the site investigators for collecting, organizing, and distributing the data required for this analysis. We thank the anonymous referee and Yiqi Luo for comments that improved the manuscript. A portion of this research was performed using PNNL Institutional Computing at Pacific Northwest National Laboratory. PNNL is operated by Battelle for the US Department of Energy under contract DE-AC05-76RL01830. NR 48 TC 0 Z9 0 U1 2 U2 9 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 2015 VL 8 IS 3 BP 781 EP 789 DI 10.5194/gmd-8-781-2015 PG 9 WC Geosciences, Multidisciplinary SC Geology GA CE9JM UT WOS:000352160200016 ER PT J AU Lebassi-Habtezion, B Caldwell, PM AF Lebassi-Habtezion, B. Caldwell, P. M. TI Aerosol specification in single-column Community Atmosphere Model version 5 SO GEOSCIENTIFIC MODEL DEVELOPMENT LA English DT Article ID SOUTHEAST PACIFIC STRATOCUMULUS; SHALLOW CUMULUS CONVECTION; MARINE STRATOCUMULUS; CLIMATE SIMULATIONS; EFFECTIVE RADIUS; BOUNDARY-LAYER; CLOUD; PARAMETERIZATION; SENSITIVITY; RADIATION AB Single-column model (SCM) capability is an important tool for general circulation model development. In this study, the SCM mode of version 5 of the Community Atmosphere Model (CAM5) is shown to handle aerosol initialization and advection improperly, resulting in aerosol, cloud-droplet, and ice crystal concentrations which are typically much lower than observed or simulated by CAM5 in global mode. This deficiency has a major impact on stratiform cloud simulations but has little impact on convective case studies because aerosol is currently not used by CAM5 convective schemes and convective cases are typically longer in duration (so initialization is less important). By imposing fixed aerosol or cloud-droplet and crystal number concentrations, the aerosol issues described above can be avoided. Sensitivity studies using these idealizations suggest that the Meyers et al. (1992) ice nucleation scheme prevents mixed-phase cloud from existing by producing too many ice crystals. Microphysics is shown to strongly deplete cloud water in stratiform cases, indicating problems with sequential splitting in CAM5 and the need for careful interpretation of output from sequentially split climate models. Droplet concentration in the general circulation model (GCM) version of CAM5 is also shown to be far too low (similar to 25 cm(-3)) at the southern Great Plains (SGP) Atmospheric Radiation Measurement (ARM) site. C1 [Lebassi-Habtezion, B.; Caldwell, P. M.] Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. RP Caldwell, PM (reprint author), Lawrence Livermore Natl Lab, POB 808, Livermore, CA 94551 USA. EM caldwell19@llnl.gov FU Lawrence Livermore National Laboratory (LLNL) through the Multiscale Scientific Discovery through Advanced Computing (SciDAC) project; United States Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07NA27344] FX We thank the Lawrence Livermore National Laboratory (LLNL) for providing funding through the Multiscale Scientific Discovery through Advanced Computing (SciDAC) project. The research was performed under the auspices of the United States Department of Energy by Lawrence Livermore National Laboratory under contract DE-AC52-07NA27344. NR 46 TC 1 Z9 1 U1 1 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 2015 VL 8 IS 3 BP 817 EP 828 DI 10.5194/gmd-8-817-2015 PG 12 WC Geosciences, Multidisciplinary SC Geology GA CE9JM UT WOS:000352160200019 ER PT J AU Nasirian, A Cortes, DD Dai, S AF Nasirian, A. Cortes, D. D. Dai, S. TI The physical nature of thermal conduction in dry granular media SO GEOTECHNIQUE LETTERS LA English DT Article DE geophysics; laboratory tests; sands ID ENERGY GEOTECHNOLOGY; HEAT-CONDUCTION; RESISTIVITY; SOILS; BEDS AB This paper documents the results of a laboratory experimental study conducted to explore the relative contributions of phonon and electron heat conduction in an electrically conductive granular material under increasing confining stresses. The thermal conductivity of Ottawa sand under increasing confinement was also studied to offer a baseline for comparison. Simultaneous measurements of thermal conductivity, electrical conductivity and p-wave velocity were used to develop a parallel conduction model capable of predicting the thermal conductivity of dry granular media. The results suggest that the thermal conductivity of dry granular media is governed by the stiffness of the packing, regardless of whether it is electrically conductive or not. Furthermore, p-wave velocity measurements can be used to estimate the thermal conductivity of electrically conductive (granular lead) and non-conductive (Ottawa sand) granular media. C1 [Nasirian, A.; Cortes, D. D.] New Mexico State Univ, Dept Civil Engn, Las Cruces, NM 88003 USA. [Dai, S.] US DOE, Natl Energy Technol Lab, Morgantown, WV USA. RP Nasirian, A (reprint author), New Mexico State Univ, Dept Civil Engn, Las Cruces, NM 88003 USA. RI Cortes, Douglas/A-7879-2013 FU College of Engineering; Civil Engineering Department of New Mexico State University FX Support for this research was provided by start-up funding from the College of Engineering and the Civil Engineering Department of New Mexico State University. NR 31 TC 3 Z9 3 U1 0 U2 15 PU ICE PUBLISHING PI WESTMINISTER PA INST CIVIL ENGINEERS, 1 GREAT GEORGE ST, WESTMINISTER SW 1P 3AA, ENGLAND SN 2049-825X EI 2045-2543 J9 GEOTECH LETT JI Geotech. Lett. PD JAN PY 2015 VL 5 IS 1 BP 1 EP 5 DI 10.1680/geolett.14.00073 PG 5 WC Engineering, Geological SC Engineering GA CF6FX UT WOS:000352653600001 ER PT J AU Harper-Slaboszewicz, VJ Leckbee, J Bennett, N Madrid, EA Rose, DV Thoma, C Welch, DR Lake, PW McCourt, AL AF Harper-Slaboszewicz, Victor J. Leckbee, Joshua Bennett, Nichelle Madrid, Elizabeth A. Rose, David V. Thoma, Carsten Welch, Dale R. Lake, Patrick W. McCourt, Andrew L. TI Parallel Operation of Multiple Closely Spaced Small Aspect Ratio Rod Pinches SO IEEE TRANSACTIONS ON PLASMA SCIENCE LA English DT Article DE Rod pinch ID PARTICLE-IN-CELL; ELECTRON FLOW; RADIOGRAPHY SOURCE; DIODE; TRANSPORT; PLASMA; MV; PROPAGATION; SIMULATION; POWER AB A series of simulations and experiments to resolve questions about the operation of arrays of closely spaced small aspect ratio rod pinches has been performed. Design and postshot analysis of the experimental results are supported by 3-D particle-in-cell simulations. Both simulations and experiments support these conclusions. Penetration of current to the interior of the array appears to be efficient, as the current on the center rods is essentially equal to the current on the outer rods. Current loss in the feed due to the formation of magnetic nulls was avoided in these experiments by design of the feed surface of the cathode and control of the gap to keep the electric fields on the cathode below the emission threshold. Some asymmetry in the electron flow to the rod was observed, but the flow appeared to symmetrize as it reached the end of the rod. Interaction between the rod pinches can be controlled to allow the stable and consistent operation of arrays of rod pinches. C1 [Harper-Slaboszewicz, Victor J.; Leckbee, Joshua; Lake, Patrick W.; McCourt, Andrew L.] Sandia Natl Labs, Albuquerque, NM 87123 USA. [Bennett, Nichelle] Natl Secur Technol LLC, Las Vegas, NV 89030 USA. [Madrid, Elizabeth A.; Rose, David V.; Thoma, Carsten; Welch, Dale R.] Voss Sci LLC, Albuquerque, NM 87108 USA. RP Harper-Slaboszewicz, VJ (reprint author), Sandia Natl Labs, Albuquerque, NM 87123 USA. EM vjharpe@sandia.gov; jjleckb@sandia.gov; nlbenne@sandia.gov; elizabethm@vosssci.com; davidr@vosssci.com; carstent@vosssci.com; dalew@vosssci.com; pwlake@sandia.gov; almccou@sandia.gov FU Laboratory Directed Research and Development Program through Sandia National Laboratories; U.S. Department of Energy within the National Nuclear Security Administration [DE-AC04-94AL85000] FX This work was supported by the Laboratory Directed Research and Development Program through Sandia National Laboratories. Sandia National Laboratories is a Multiprogram Laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, through the U.S. Department of Energy within the National Nuclear Security Administration under Contract DE-AC04-94AL85000. NR 23 TC 0 Z9 0 U1 3 U2 3 PU IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC PI PISCATAWAY PA 445 HOES LANE, PISCATAWAY, NJ 08855-4141 USA SN 0093-3813 EI 1939-9375 J9 IEEE T PLASMA SCI JI IEEE Trans. Plasma Sci. PD JAN PY 2015 VL 43 IS 1 BP 422 EP 432 DI 10.1109/TPS.2014.2376272 PN 3 PG 11 WC Physics, Fluids & Plasmas SC Physics GA CE8HQ UT WOS:000352083000006 ER PT S AU Ivanshin, VA Litvinova, TO Gimranova, K Sukhanov, AA Jia, S Bud'ko, SL Canfield, PC AF Ivanshin, V. A. Litvinova, T. O. Gimranova, K. Sukhanov, A. A. Jia, S. Bud'ko, S. L. Canfield, P. C. BE Zhitomirsky, M DeReotier, PD TI Dual nature of 3d electrons in YbT2Zn20 (T = Co; Fe) evidenced by electron spin resonance SO INTERNATIONAL CONFERENCE ON STRONGLY CORRELATED ELECTRON SYSTEMS 2014 (SCES2014) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT International Conference on Strongly Correlated Electron Systems (SCES) CY JUL 07-14, 2014 CL Univ Grenoble, Grenoble, FRANCE HO Univ Grenoble ID COMPOUND; IR AB The electron spin resonance experiments were carried out in the single crystals YbFe2Zn20. The observed spin dynamics is compared with that in YbFe2Zn20 and YbFe2Zn20 as well as with the data of inelastic neutron scattering and electronic band structure calculations. Our results provide direct evidence that 3d electrons are itinerant in YbFe2Zn20 and localized in YbFe2Zn20. Possible connection between spin paramagnetism of dense heavy fermion systems, quantum criticality effects, and ESR spectra is discussed. C1 [Ivanshin, V. A.; Litvinova, T. O.; Gimranova, K.] Kazan Volga Reg Fed Univ, Kazan 420008, Russia. [Sukhanov, A. A.] Zavoisky Phys Tech Inst, Kazan 420029, Russia. [Jia, S.; Bud'ko, S. L.; Canfield, P. C.] Iowa State Univ, Ames Lab, US DOE, Ames, IA 50011 USA. [Jia, S.; Bud'ko, S. L.; Canfield, P. C.] Iowa State Univ, Dept Phys & Astron, Ames, IA 50011 USA. RP Ivanshin, VA (reprint author), Kazan Volga Reg Fed Univ, Kremlevskaya Str 18, Kazan 420008, Russia. EM Vladimir.Ivanshin@kpfu.ru OI Sukhanov, Andrey/0000-0001-8927-3715 NR 25 TC 0 Z9 0 U1 0 U2 6 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2015 VL 592 AR 012084 DI 10.1088/1742-6596/592/1/012084 PG 6 WC Physics, Atomic, Molecular & Chemical; Physics, Multidisciplinary SC Physics GA BC4BG UT WOS:000352239200084 ER PT S AU Jeffries, JR Butch, NP Vohra, YK Weir, ST AF Jeffries, J. R. Butch, N. P. Vohra, Y. K. Weir, S. T. BE Zhitomirsky, M DeReotier, PD TI Pressure evolution of electrical transport in the 3D topological insulator (Bi,Sb)(2)(Se,Te)(3) SO INTERNATIONAL CONFERENCE ON STRONGLY CORRELATED ELECTRON SYSTEMS 2014 (SCES2014) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT International Conference on Strongly Correlated Electron Systems (SCES) CY JUL 07-14, 2014 CL Univ Grenoble, Grenoble, FRANCE HO Univ Grenoble ID SB2TE3 AB The group V-VI compounds-like Bi2Se3, Sb2Te3, or Bi2Te3-have been widely studied in recent years for their bulk topological properties. The high-Z members of this series form with the same crystal structure, and are therefore amenable to isostructural substitution studies. It is possible to tune the Bi-Sb and Te-Se ratios such that the material exhibits insulating behavior, thus providing an excellent platform for understanding how a topological insulator evolves with applied pressure. We report our observations of the pressure-dependent electrical transport and crystal structure of a pseudobinary (Bi, Sb)(2)(Te, Se)(3) compound. Similar to some of its sister compounds, the (Bi, Sb)(2)(Te, Se)(3) pseudobinary compound undergoes multiple, pressure-induced phase transformations that result in metallization, the onset of a close-packed crystal structure, and the development of distinct superconducting phases. C1 [Jeffries, J. R.; Butch, N. P.; Weir, S. T.] Lawrence Livermore Natl Lab, Condensed Matter & Mat Div, Livermore, CA 94550 USA. [Butch, N. P.] NIST, Ctr Neutron Res, Gaithersburg, MD 20899 USA. [Vohra, Y. K.] Univ Alabama Birmingham, Dept Phys, Birmingham, AL 35294 USA. RP Jeffries, JR (reprint author), Lawrence Livermore Natl Lab, Condensed Matter & Mat Div, Livermore, CA 94550 USA. EM jeffries4@llnl.gov NR 16 TC 0 Z9 0 U1 4 U2 19 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2015 VL 592 AR 012124 DI 10.1088/1742-6596/592/1/012124 PG 5 WC Physics, Atomic, Molecular & Chemical; Physics, Multidisciplinary SC Physics GA BC4BG UT WOS:000352239200124 ER PT S AU Okamura, H Takigawa, A Bauer, ED Moriwaki, T Ikemoto, Y AF Okamura, H. Takigawa, A. Bauer, E. D. Moriwaki, T. Ikemoto, Y. BE Zhitomirsky, M DeReotier, PD TI Pressure evolution of f electron hybridized state in CeCoIn5 studied by optical conductivity SO INTERNATIONAL CONFERENCE ON STRONGLY CORRELATED ELECTRON SYSTEMS 2014 (SCES2014) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT International Conference on Strongly Correlated Electron Systems (SCES) CY JUL 07-14, 2014 CL Univ Grenoble, Grenoble, FRANCE HO Univ Grenoble AB Optical conductivity sigma(omega) of CeCoIn5 has been measured under high pressure to 8 GPa and at low temperatures to 6 K, to study the pressure evolution of the conduction (c)-f electron hybridized state near the Fermi level. At ambient pressure, CeCoIn5 is a heavy fermion superconductor with T-c=2.3 K, and has moderately strong c-f hybridization. sigma(omega) at ambient pressure shows a marked infrared peak due to optical excitations involving the c-f hybridized state. With increasing pressure, the infrared peak becomes broader, and its center shifts to higher energy. This result indicates that the large density of states of the c-f hybridized state becomes broader with increasing pressure, and that the peak of the density of states shifts away from the Fermi level. Althouth such pressure evolution of the c-f hybridized state had been widely assumed on the basis of theoretical consideration, the present optical result demonstrates it clearly and directly. C1 [Okamura, H.; Takigawa, A.] Kobe Univ, Grad Sch Sci, Dept Phys, Kobe, Hyogo 6578501, Japan. [Bauer, E. D.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Moriwaki, T.; Ikemoto, Y.] Japan Synchrotron Radiat Res Inst, Sayo 6795198, Japan. RP Okamura, H (reprint author), Kobe Univ, Grad Sch Sci, Dept Phys, Kobe, Hyogo 6578501, Japan. EM okamura@kobe-u.ac.jp OI Bauer, Eric/0000-0003-0017-1937 NR 22 TC 3 Z9 3 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 2015 VL 592 AR 012001 DI 10.1088/1742-6596/592/1/012001 PG 5 WC Physics, Atomic, Molecular & Chemical; Physics, Multidisciplinary SC Physics GA BC4BG UT WOS:000352239200001 ER PT S AU Ronning, F Zhu, JX AF Ronning, F. Zhu, J. -X. BE Zhitomirsky, M DeReotier, PD TI Electronic structure of U2PtC2 and U2RhC2 SO INTERNATIONAL CONFERENCE ON STRONGLY CORRELATED ELECTRON SYSTEMS 2014 (SCES2014) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT International Conference on Strongly Correlated Electron Systems (SCES) CY JUL 07-14, 2014 CL Univ Grenoble, Grenoble, FRANCE HO Univ Grenoble ID HEAVY FERMIONS; SYSTEMS; CARBIDES AB We present density functional theory calculations within the generalized gradient approximation of U2RhC2 and U2PtC2. We find the calculated density of states are significantly less than that measured by specific heat indicating the need for electronic correlations. The mass enhancement found for U2PtC2 is m*/m(band) approximate to 4. C1 [Ronning, F.; Zhu, J. -X.] Los Alamos Natl Lab, Los Alamos, NM 87544 USA. RP Ronning, F (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87544 USA. EM fronning@lanl.gov OI Ronning, Filip/0000-0002-2679-7957 NR 21 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 2015 VL 592 AR 012037 DI 10.1088/1742-6596/592/1/012037 PG 5 WC Physics, Atomic, Molecular & Chemical; Physics, Multidisciplinary SC Physics GA BC4BG UT WOS:000352239200037 ER PT S AU Schaab, J Trassin, M Scholl, A Doran, A Yan, Z Bourret, E Ramesh, R Meier, D AF Schaab, J. Trassin, M. Scholl, A. Doran, A. Yan, Z. Bourret, E. Ramesh, R. Meier, D. BE Zhitomirsky, M DeReotier, PD TI Ferroelectric domains in the multiferroic phase of ErMnO3 imaged by low-temperature photoemission electron microscopy SO INTERNATIONAL CONFERENCE ON STRONGLY CORRELATED ELECTRON SYSTEMS 2014 (SCES2014) SE Journal of Physics Conference Series LA English DT Proceedings Paper CT International Conference on Strongly Correlated Electron Systems (SCES) CY JUL 07-14, 2014 CL Univ Grenoble, Grenoble, FRANCE HO Univ Grenoble ID WALLS; YMNO3; MANGANITE AB Low-temperature photoemission electron microscopy (PEEM) is used to image and compare the distribution of ferroelectric domains in multiferroic ErMnO3 above and below the magnetic ordering temperature (T-N = 80 K). Our temperature-dependent PEEM data demonstrate that the ferroelectric domain structure is robust against the onset of magnetic long-range order and the emergence of antiferromagnetic domains. The observed persistence indicates that antiferromagnetic domain walls adopt the position of ferroelectric walls - and not vice versa - developing a multiferroic domain-wall pattern congruent with the ferroelectric domain-wall distribution observed above T-N. C1 [Schaab, J.; Trassin, M.; Meier, D.] ETH, Dept Mat, CH-8093 Zurich, Switzerland. [Scholl, A.; Doran, A.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. [Yan, Z.; Bourret, E.; Ramesh, R.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. [Ramesh, R.] Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. RP Schaab, J (reprint author), ETH, Dept Mat, CH-8093 Zurich, Switzerland. EM dennis.meier@mat.ethz.ch RI Scholl, Andreas/K-4876-2012 NR 26 TC 1 Z9 1 U1 4 U2 43 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2015 VL 592 AR 012120 DI 10.1088/1742-6596/592/1/012120 PG 5 WC Physics, Atomic, Molecular & Chemical; Physics, Multidisciplinary SC Physics GA BC4BG UT WOS:000352239200120 ER PT J AU Stoyanov, M Webster, CG AF Stoyanov, M. Webster, C. G. TI A GRADIENT-BASED SAMPLING APPROACH FOR DIMENSION REDUCTION OF PARTIAL DIFFERENTIAL EQUATIONS WITH STOCHASTIC COEFFICIENTS SO INTERNATIONAL JOURNAL FOR UNCERTAINTY QUANTIFICATION LA English DT Article DE representation of uncertainty; stochastic model reduction method; stochastic sensitivity analysis; high-dimensional approximation; stochastic partial differential equations; Karhunen-Loeve expansion; Monte Carlo ID RANDOM INPUT DATA; COLLOCATION METHOD; SPARSE; INTERPOLATION; UNCERTAINTY AB We develop a projection-based dimension reduction approach for partial differential equations with high-dimensional stochastic coefficients. This technique uses samples of the gradient of the quantity of interest (QoI) to partition the uncertainty domain into "active" and "passive" subspaces. The passive subspace is characterized by near-constant behavior of the quantity of interest, while the active subspace contains the most important dynamics of the stochastic system. We also present a procedure to project the model onto the low-dimensional active subspace that enables the resulting approximation to be solved using conventional techniques. Unlike the classical Karhunen-Loeve expansion, the advantage of this approach is that it is applicable to fully nonlinear problems and does not require any assumptions on the correlation between the random inputs. This work also provides a rigorous convergence analysis of the quantity of interest and demonstrates: at least linear convergence with respect to the number of samples. It also shows that the convergence rate is independent of the number of input random variables. Thus, applied to a reducible problem, our approach can approximate the statistics of the QoI to within desired error tolerance at a cost that is orders of magnitude lower than standard Monte Carlo. Finally, several numerical examples demonstrate the feasibility of our approach and are used to illustrate the theoretical results. In particular, we validate our convergence estimates through the application of this approach to a reactor criticality problem with a large number of random cross-section parameters. C1 [Stoyanov, M.; Webster, C. G.] Oak Ridge Natl Lab, Comp Sci & Math Div, Appl Math Grp, Oak Ridge, TN 37831 USA. RP Webster, CG (reprint author), Oak Ridge Natl Lab, Comp Sci & Math Div, Appl Math Grp, 1 Bethel Valley Rd,POB 2008, Oak Ridge, TN 37831 USA. EM webstercg@ornl.gov FU Office of Science of the US Department of Energy [ERKJE45]; US Air Force Office of Scientific Research [1854-V521-12]; Lab- oratory Directed Research and Development program at the Oak Ridge National Laboratory (ORNL); US Department of Energy [DE-AC05-00OR22725] FX The preparation of the article was supported in part by the Office of Science of the US Department of Energy under grant number ERKJE45; by the US Air Force Office of Scientific Research under grant number 1854-V521-12; and by the Lab- oratory Directed Research and Development program at the Oak Ridge National Laboratory (ORNL). The ORNL is operated by UT-Battelle, LLC, for the US Department of Energy under Contract DE-AC05-00OR22725. NR 35 TC 1 Z9 1 U1 0 U2 0 PU BEGELL HOUSE INC PI DANBURY PA 50 NORTH ST, DANBURY, CT 06810 USA SN 2152-5080 EI 2152-5099 J9 INT J UNCERTAIN QUAN JI Int. J. Uncertain. Quantif. PY 2015 VL 5 IS 1 BP 49 EP 72 DI 10.1615/Int.J.UncertaintyQuantification.2014010945 PG 24 WC Engineering, Multidisciplinary; Mathematics, Interdisciplinary Applications SC Engineering; Mathematics GA CF6YB UT WOS:000352701700003 ER PT J AU Devan, RS Ma, YR Kim, JH Bhattacharya, RN Ghosh, KC AF Devan, Rupesh S. Ma, Yuan-Ron Kim, Jin-Hyeok Bhattacharya, Raghu N. Ghosh, Kartik C. TI Functional Nanomaterials for Energy Applications SO JOURNAL OF NANOMATERIALS LA English DT Editorial Material C1 [Devan, Rupesh S.] Univ Pune, Dept Phys, Pune 411007, Maharashtra, India. [Ma, Yuan-Ron] Natl Dong Hwa Univ, Dept Phys, Hualien 97401, Taiwan. [Kim, Jin-Hyeok] Chonnam Natl Univ, Dept Mat Sci & Engn, Gwangju 500757, South Korea. [Bhattacharya, Raghu N.] Natl Renewable Energy Lab, Golden, CO 80401 USA. [Ghosh, Kartik C.] SW Missouri State Univ, Dept Phys Astron & Mat Sci, Springfield, MO 65897 USA. RP Devan, RS (reprint author), Univ Pune, Dept Phys, Pune 411007, Maharashtra, India. EM devan_rs@yahoo.co.in; ronma@mail.ndhu.edu.tw RI Devan, Rupesh/E-1883-2011 OI Devan, Rupesh/0000-0001-9550-7506 NR 0 TC 0 Z9 0 U1 1 U2 5 PU HINDAWI PUBLISHING CORPORATION PI NEW YORK PA 410 PARK AVENUE, 15TH FLOOR, #287 PMB, NEW YORK, NY 10022 USA SN 1687-4110 EI 1687-4129 J9 J NANOMATER JI J. Nanomater. PY 2015 AR 131965 DI 10.1155/2015/131965 PG 2 WC Nanoscience & Nanotechnology; Materials Science, Multidisciplinary SC Science & Technology - Other Topics; Materials Science GA CF2XM UT WOS:000352411100001 ER PT J AU Millet, LJ Lucheon, JD Standaert, RF Retterer, ST Doktycz, MJ AF Millet, L. J. Lucheon, J. D. Standaert, R. F. Retterer, S. T. Doktycz, M. J. TI Modular microfluidics for point-of-care protein purifications SO LAB ON A CHIP LA English DT Article ID LIQUID-CHROMATOGRAPHY; MASS-SPECTROMETRY; DRUG DISCOVERY; SEPARATION; DEVICE; SYSTEMS; EXPRESSION; SELECTION; NEURONS; BINDING AB Biochemical separations are the heart of diagnostic assays and purification methods for biologics. On-chip miniaturization and modularization of separation procedures will enable the development of customized, portable devices for personalized health-care diagnostics and point-of-use production of treatments. In this report, we describe the design and fabrication of miniature ion exchange, size exclusion and affinity chromatography modules for on-chip clean-up of recombinantly-produced proteins. Our results demonstrate that these common separations techniques can be implemented in microfluidic modules with performance comparable to conventional approaches. We introduce embedded 3-D microfluidic interconnects for integrating micro-scale separation modules that can be arranged and reconfigured to suit a variety of fluidic operations or biochemical processes. We demonstrate the utility of the modular approach with a platform for the enrichment of enhanced green fluorescent protein (eGFP) from Escherichia coli lysate through integrated affinity and size-exclusion chromatography modules. C1 [Millet, L. J.; Lucheon, J. D.; Standaert, R. F.; Retterer, S. T.; Doktycz, M. J.] Oak Ridge Natl Lab, Biosci Div, Biol & Nanoscale Syst Grp, Oak Ridge, TN 37831 USA. [Millet, L. J.; Standaert, R. F.; Retterer, S. T.; Doktycz, M. J.] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. RP Millet, LJ (reprint author), Oak Ridge Natl Lab, Biosci Div, Biol & Nanoscale Syst Grp, POB 2008 MS 6445, Oak Ridge, TN 37831 USA. EM milletlj@ornl.gov RI Retterer, Scott/A-5256-2011; Standaert, Robert/D-9467-2013; Doktycz, Mitchel/A-7499-2011; OI Retterer, Scott/0000-0001-8534-1979; Standaert, Robert/0000-0002-5684-1322; Doktycz, Mitchel/0000-0003-4856-8343; Millet, Larry /0000-0001-6443-2505 FU DARPA award [HR001134005]; UT-Battelle, LLC [DE-AC05-00OR22725]; Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy FX We express gratitude and appreciation to Carmen Foster, Stephen Foster, and Cathy Gaudreau for their assistance and administrative support. We express appreciation to John Dresios and Henri Sasmore at Leidos for helpful discussions. This work was supported by DARPA award HR001134005. The views expressed are those of the authors and do not reflect the official policy or position of the Department of Defense or the U.S. Government. This research was performed at Oak Ridge National Laboratory (ORNL). ORNL is managed by UT-Battelle, LLC, for the US Department of Energy Under contract DE-AC05-00OR22725. 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 38 TC 8 Z9 8 U1 9 U2 55 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1473-0197 EI 1473-0189 J9 LAB CHIP JI Lab Chip PY 2015 VL 15 IS 8 BP 1799 EP 1811 DI 10.1039/c5lc00094g PG 13 WC Biochemical Research Methods; Chemistry, Multidisciplinary; Nanoscience & Nanotechnology SC Biochemistry & Molecular Biology; Chemistry; Science & Technology - Other Topics GA CE8JM UT WOS:000352088400002 PM 25740172 ER PT J AU Nallathamby, PD Mortensen, NP Palko, HA Malfatti, M Smith, C Sonnett, J Doktycz, MJ Gu, BH Roeder, RK Wang, W Retterer, ST AF Nallathamby, Prakash D. Mortensen, Ninell P. Palko, Heather A. Malfatti, Mike Smith, Catherine Sonnett, James Doktycz, Mitchel J. Gu, Baohua Roeder, Ryan K. Wang, Wei Retterer, Scott T. TI New surface radiolabeling schemes of super paramagnetic iron oxide nanoparticles (SPIONs) for biodistribution studies SO NANOSCALE LA English DT Article ID ACCELERATOR MASS-SPECTROMETRY; IN-VITRO; DRUG-DELIVERY; MAGNETIC NANOPARTICLES; CANCER-THERAPY; TOXICITY; DESIGN; CELLS; LUNG; PHARMACOKINETICS AB Nanomaterial based drug delivery systems allow for the independent tuning of the surface chemical and physical properties that affect their biodistribution in vivo and the therapeutic payloads that they are intended to deliver. Additionally, the added therapeutic and diagnostic value of their inherent material properties often provides extra functionality. Iron based nanomaterials with their magnetic properties and easily tailorable surface chemistry are of particular interest as model systems. In this study the core radius of the iron oxide nanoparticles (NPs) was 14.08 +/- 3.92 nm while the hydrodynamic radius of the NPs, as determined by Dynamic Light Scattering (DLS), was between 90-110 nm. In this study, different approaches were explored to create radiolabeled NPs that are stable in solution. The NPs were functionalized with polycarboxylate or polyamine surface functional groups. Polycarboxylate functionalized NPs had a zeta potential of -35 mV and polyamine functionalized NPs had a zeta potential of +40 mV. The polycarboxylate functionalized NPs were chosen for in vivo biodistribution studies and hence were radiolabeled with C-14, with a final activity of 0.097 nCi mg(-1) of NPs. In chronic studies, the biodistribution profile is tracked using low level radiolabeled proxies of the nanoparticles of interest. Conventionally, these radiolabeled proxies are chemically similar but not chemically identical to the non-radiolabeled NPs of interest. This study is novel as different approaches were explored to create radiolabeled NPs that are stable, possess a hydrodynamic radius of <100 nm and most importantly they exhibit an identical surface chemical functionality as their non-radiolabeled counterparts. Identical chemical functionality of the radiolabeled probes to the non-radiolabeled probes was an important consideration to generate statistically similar biodistribution data sets using multiple imaging and detection techniques. The radiolabeling approach described here is applicable to the synthesis of a large class of nanomaterials with multiple core and surface functionalities. This work combined with the biodistribution data suggests that the radiolabeling schemes carried out in this study have broad implications for use in pharmacokinetic studies for a variety of nanomaterials. C1 [Nallathamby, Prakash D.; Palko, Heather A.; Smith, Catherine; Sonnett, James] Battelle Mem Inst, Battelle Ctr Fundamental & Appl Syst Toxicol, Columbus, OH 43201 USA. [Nallathamby, Prakash D.; Mortensen, Ninell P.; Doktycz, Mitchel J.; Gu, Baohua; Wang, Wei; Retterer, Scott T.] Oak Ridge Natl Lab, Biol & Environm Sci Div, Oak Ridge, TN 37831 USA. [Palko, Heather A.; Malfatti, Mike] Lawrence Livermore Natl Lab, Phys & Life Sci, Biosci & Biotechnol Div, Livermore, CA 94550 USA. [Nallathamby, Prakash D.; Roeder, Ryan K.] Univ Notre Dame, Dept Aerosp & Mech Engn, Bioengn Grad Program, Notre Dame, IN 46556 USA. RP Nallathamby, PD (reprint author), Battelle Mem Inst, Battelle Ctr Fundamental & Appl Syst Toxicol, 505 King Ave, Columbus, OH 43201 USA. EM pnallath@nd.edu; wangw@ornl.gov; rettererst@ornl.gov RI Roeder, Ryan/A-9398-2008; Wang, Wei/B-5924-2012; Retterer, Scott/A-5256-2011; Gu, Baohua/B-9511-2012; Doktycz, Mitchel/A-7499-2011 OI Roeder, Ryan/0000-0003-1576-6570; Retterer, Scott/0000-0001-8534-1979; Gu, Baohua/0000-0002-7299-2956; Doktycz, Mitchel/0000-0003-4856-8343 FU B-FAST, Battelle Center for Fundamental and Applied Systems Toxicology, Multi-Scale Toxicity Initiative; U.S. Department of Energy [DE-AC05-00OR22725]; Division of Scientific User Facilities; NSF [DMR-1309587] FX This research was supported by the B-FAST, Battelle Center for Fundamental and Applied Systems Toxicology, Multi-Scale Toxicity Initiative. This manuscript has been authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. Dr. Nallathamby would like to acknowledge material support through proposal #CNMS2013-153, from the Center for Nanophase Materials Sciences, which is sponsored at Oak Ridge National Laboratory by the Division of Scientific User Facilities. We acknowledge the Notre Dame Integrated Imaging Facility (NDIFF) for the use of transmission electron microscopy. Instrument time at NDIIF was funded by Dr. Roeder through NSF DMR-1309587. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan http://energy.gov/downloads/doe-public-access-plan. NR 58 TC 7 Z9 7 U1 4 U2 28 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2040-3364 EI 2040-3372 J9 NANOSCALE JI Nanoscale PY 2015 VL 7 IS 15 BP 6545 EP 6555 DI 10.1039/c4nr06441k PG 11 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA CF1BC UT WOS:000352277500020 PM 25790032 ER PT J AU Guillot, SL Mistry, KS Avery, AD Richard, J Dowgiallo, AM Ndione, PF van de Lagemaat, J Reese, MO Blackburn, JL AF Guillot, Sarah L. Mistry, Kevin S. Avery, Azure D. Richard, Jonah Dowgiallo, Anne-Marie Ndione, Paul F. van de Lagemaat, Jao Reese, Matthew O. Blackburn, Jeffrey L. TI Precision printing and optical modeling of ultrathin SWCNT/C-60 heterojunction solar cells SO NANOSCALE LA English DT Article ID WALLED CARBON NANOTUBES; THIN-FILM PHOTOVOLTAICS; QUANTUM EFFICIENCY; EXCITON DIFFUSION; CHARGE GENERATION; TRANSPARENT; TRANSISTORS; COMPOSITES; ELEMENTS; SPECTRA AB Semiconducting single-walled carbon nanotubes (s-SWCNTs) are promising candidates as the active layer in photovoltaics (PV), particularly for niche applications where high infrared absorbance and/or semi-transparent solar cells are desirable. Most current fabrication strategies for SWCNT PV devices suffer from relatively high surface roughness and lack nanometer-scale deposition precision, both of which may hamper the reproducible production of ultrathin devices. Additionally, detailed optical models of SWCNT PV devices are lacking, due in part to a lack of well-defined optical constants for high-purity s-SWCNT thin films. Here, we present an optical model that accurately reconstructs the shape and magnitude of spectrally resolved external quantum efficiencies for ultrathin (7,5) s-SWCNT/C-60 solar cells that are deposited by ultrasonic spraying. The ultrasonic spraying technique enables thickness tuning of the s-SWCNT layer with nanometer-scale precision, and consistently produces devices with low s-SWCNT film average surface roughness (R-q of <5 nm). Our optical model, based entirely on measured optical constants of each layer within the device stack, enables quantitative predictions of thickness-dependent relative photocurrent contributions of SWCNTs and C-60 and enables estimates of the exciton diffusion lengths within each layer. These results establish routes towards rational performance improvements and scalable fabrication processes for ultra-thin SWCNT-based solar cells. C1 [Guillot, Sarah L.] Univ Wisconsin, Madison, WI USA. [Mistry, Kevin S.; Avery, Azure D.; Richard, Jonah; Dowgiallo, Anne-Marie; Ndione, Paul F.; van de Lagemaat, Jao; Reese, Matthew O.; Blackburn, Jeffrey L.] Natl Renewable Energy Lab, Golden, CO 80401 USA. RP Blackburn, JL (reprint author), Natl Renewable Energy Lab, Golden, CO 80401 USA. EM Jeffrey.Blackburn@nrel.gov RI van de Lagemaat, Jao/J-9431-2012; Ndione, Paul/O-6152-2015; OI Ndione, Paul/0000-0003-4444-2938; Guillot, Sarah/0000-0003-0887-897X FU NREL's Laboratory Directed Research and Development (LDRD) program FX This work was funded by the NREL's Laboratory Directed Research and Development (LDRD) program. NR 41 TC 13 Z9 13 U1 6 U2 35 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2040-3364 EI 2040-3372 J9 NANOSCALE JI Nanoscale PY 2015 VL 7 IS 15 BP 6556 EP 6566 DI 10.1039/c5nr00205b PG 11 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA CF1BC UT WOS:000352277500021 PM 25790468 ER PT J AU Lucena, AF Lourenco, C Michelini, MC Rutkowski, PX Carretas, JM Zorz, N Berthon, L Dias, A Oliveira, MC Gibson, JK Marcalo, J AF Lucena, Ana F. Lourenco, Celia Michelini, Maria C. Rutkowski, Philip X. Carretas, Jose M. Zorz, Nicole Berthon, Laurence Dias, Ana Conceicao Oliveira, M. Gibson, John K. Marcalo, Joaquim TI Synthesis and hydrolysis of gas-phase lanthanide and actinide oxide nitrate complexes: a correspondence to trivalent metal ion redox potentials and ionization energies SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID STANDARD ELECTRODE-POTENTIALS; THERMAL-DECOMPOSITION; SPRAY-PYROLYSIS; NICKEL NITRATE; THERMODYNAMIC PREDICTIONS; MASS-SPECTROMETRY; OXIDATION-STATES; BASIS-SETS; AQUO IONS; HEXAHYDRATE AB Several lanthanide and actinide tetranitrate ions, M-III(NO3)(4)(-), were produced by electrospray ionization and subjected to collision induced dissociation in quadrupole ion trap mass spectrometers. The nature of the MO(NO3)(3)(-)products that result from NO2 elimination was evaluated by measuring the relative hydrolysis rates under thermalized conditions. Based on the experimental results it is inferred that the hydrolysis rates relate to the intrinsic stability of the M-IV oxidation states, which correlate with both the solution IV/III reduction potentials and the fourth ionization energies. Density functional theory computations of the energetics of hydrolysis and atoms-in-molecules bonding analysis of representative oxide and hydroxide nitrates substantiate the interpretations. The results allow differentiation between those MO(NO3)(3)(-) that comprise an O2- ligand with oxidation to M-IV and those that comprise a radical O- ligand with retention of the M-III oxidation state. In the particular cases of MO(NO3)(3)(-) for M = Pr, Nd and Tb it is proposed that the oxidation states are intermediate between M(III) and M(IV). C1 [Lucena, Ana F.; Lourenco, Celia; Carretas, Jose M.; Marcalo, Joaquim] Univ Lisbon, Inst Super Tecn, Ctr Ciencias & Tecnol Nucl, P-2695066 Bobadela Lrs, Portugal. [Michelini, Maria C.] Univ Calabria, Dipartimento Chim, I-87030 Arcavacata Di Rende, Italy. [Rutkowski, Philip X.; Gibson, John K.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. [Zorz, Nicole; Berthon, Laurence] CEA, Nucl Energy Div, Radiochem & Proc Dept, Lab Ligands Actinides Interact, F-30207 Bagnols Sur Ceze, France. [Dias, Ana; Conceicao Oliveira, M.] Univ Lisbon, Inst Super Tecn, Ctr Quim Estrutural, P-1049001 Lisbon, Portugal. RP Michelini, MC (reprint author), Univ Calabria, Dipartimento Chim, I-87030 Arcavacata Di Rende, Italy. EM mc.michelini@unical.it; jmarcalo@ctn.ist.utl.pt RI BERTHON, Laurence/B-1374-2016; PTMS, RNEM/C-1589-2014; Marcalo, Joaquim/J-5476-2013; OI BERTHON, Laurence/0000-0003-3474-8474; Marcalo, Joaquim/0000-0001-7580-057X; Lourenco, Celia/0000-0002-2323-3304 FU Fundacao para a Ciencia e a Tecnologia [SFRH/BD/70475/2010, PTDC/QUI-QUI/108977/2008, PEst-OE/QUI/UI0100/2011]; European Commission [ACSEPT - FP7-Euratom/CP-2007-211267, ACTINET-I3-FP7-III-232631/JRP17]; Universita della Calabria; U.S. Department of Energy, Office of Basic Energy Sciences, Heavy Element Chemistry, at LBNL [DE-AC02-05CH11231]; Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]; DISN/RSTB/RBPCH (Basic Research for Physical Chemistry) Program FX This work was supported by Fundacao para a Ciencia e a Tecnologia (PhD grant SFRH/BD/70475/2010 to A.F.L.; RNEM - Rede Nacional de Espectrometria de Massa: C2TN-IST and CQE-IST Nodes; projects PTDC/QUI-QUI/108977/2008 and PEst-OE/QUI/UI0100/2011); European Commission (projects ACSEPT - FP7-Euratom/CP-2007-211267 and ACTINET-I3-FP7-III-232631/JRP17). The work of MCM was supported by Universita della Calabria. The work of PXR and JKG was fully supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Heavy Element Chemistry, at LBNL under Contract No. DE-AC02-05CH11231. This research used resources of the National Energy Research Scientific Computing Center (NERSC), which is supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. The work at the CEA was supported by the DISN/RSTB/RBPCH (Basic Research for Physical Chemistry) Program. NR 56 TC 5 Z9 5 U1 9 U2 45 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2015 VL 17 IS 15 BP 9942 EP 9950 DI 10.1039/c5cp00515a PG 9 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA CF0YN UT WOS:000352270700039 PM 25783464 ER PT J AU Thevamaran, R Karakaya, M Meshot, ER Fischer, A Podila, R Rao, AM Daraio, C AF Thevamaran, Ramathasan Karakaya, Mehmet Meshot, Eric R. Fischer, Andre Podila, Ramakrishna Rao, Apparao M. Daraio, Chiara TI Anomalous impact and strain responses in helical carbon nanotube foams SO RSC ADVANCES LA English DT Article ID MECHANICAL-PROPERTIES; TUBULE NANOCOILS; ARRAYS AB We describe the quasistatic and dynamic response of helical carbon nanotube (HCNT) foams in compression. Similarly to other CNT foams, HCNT foams exhibit preconditioning effects in response to cyclic loading; however, their fundamental deformation mechanisms are unique. In quasistatic compression, HCNT foams exhibit strain localization and collective structural buckling, nucleating at different weak sections throughout their thickness. In dynamic compression, they undergo progressive crushing, governed by the intrinsic density gradient along the thickness of the sample. HCNT microbundles often undergo brittle fracture that originates from nanoscale defects. Regardless of this microstructural damage, bulk HCNT foams exhibit super-compressibility and recover more than 90% of large compressive strains (up to 80%). When subjected to striker impacts, HCNT foams mitigate impact stresses more effectively compared to other CNT foams comprised of non-helical CNTs (similar to 50% improvement). The unique mechanical properties we revealed demonstrate that the HCNT foams are ideally suited for applications in packaging, impact protection, and vibration mitigation. C1 [Thevamaran, Ramathasan; Daraio, Chiara] CALTECH, Div Engn & Appl Sci, Pasadena, CA 91125 USA. [Thevamaran, Ramathasan; Fischer, Andre; Daraio, Chiara] ETH, Dept Mech & Proc Engn, Swiss Fed Inst Technol Zurich, CH-8092 Zurich, Switzerland. [Karakaya, Mehmet; Podila, Ramakrishna; Rao, Apparao M.] Clemson Univ, Dept Phys & Astron, Clemson, SC 29634 USA. [Karakaya, Mehmet; Podila, Ramakrishna; Rao, Apparao M.] Clemson Univ, Clemson Nanomat Ctr, Clemson, SC 29634 USA. [Meshot, Eric R.] Lawrence Livermore Natl Lab, Phys & Life Sci Directorate, Livermore, CA 94551 USA. RP Daraio, C (reprint author), CALTECH, Div Engn & Appl Sci, Pasadena, CA 91125 USA. EM daraio@ethz.ch RI Daraio, Chiara/N-2170-2015 OI Daraio, Chiara/0000-0001-5296-4440 FU Institute for Collaborative Biotechnologies (ICB) [W911NF-09-D-0001]; Army Research Office (ARO); U.S. Department of Energy by Lawrence Livermore National Laboratory [DE-AC02-05CH11231]; Office of Science, and Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231] FX We acknowledge Fabian Gramm (ScopeM, ETH Zurich) for assistance in TEM imaging and Jan Rys (ETH Zurich) for assistance in SEM imaging. We acknowledge financial support from the Institute for Collaborative Biotechnologies (ICB) under the contract W911NF-09-D-0001 with the Army Research Office (ARO). A portion of this work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344. X-ray characterization was performed at beamline 7.3.3 at the Advanced Light Source, which is supported by the Director, Office of Science, and Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract no. DE-AC02-05CH11231. NR 29 TC 1 Z9 1 U1 2 U2 6 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2046-2069 J9 RSC ADV JI RSC Adv. PY 2015 VL 5 IS 37 BP 29306 EP 29311 DI 10.1039/c5ra03561a PG 6 WC Chemistry, Multidisciplinary SC Chemistry GA CE8KQ UT WOS:000352091600062 ER PT J AU Mccourt, M Smith, B Zhang, H AF Mccourt, Michael Smith, Barry Zhang, Hong TI SPARSE MATRIX-MATRIX PRODUCTS EXECUTED THROUGH COLORING SO SIAM JOURNAL ON MATRIX ANALYSIS AND APPLICATIONS LA English DT Article DE sparse matrix product; coloring AB Sparse matrix-matrix products appear in multigrid solvers among other applications. Some implementations of these products require the inner product of two sparse vectors. In this paper, we propose a new algorithm for computing sparse matrix-matrix products by exploiting their nonzero structure through the process of graph coloring. We prove the validity of this technique in general and demonstrate its viability for examples including multigrid methods used to solve boundary value problems as well as matrix products appearing in unstructured applications. C1 [Mccourt, Michael; Smith, Barry; Zhang, Hong] Argonne Natl Lab, Div Math & Comp Sci, Argonne, IL 60439 USA. RP Mccourt, M (reprint author), Argonne Natl Lab, Div Math & Comp Sci, 9700 S Cass Ave, Argonne, IL 60439 USA. EM mccomic@mcs.anl.gov; bsmith@mcs.anl.gov; hzhang@mcs.anl.gov FU Office of Advanced Scientific Computing Research, Office of Science, U.S. Department of Energy [DE-AC02-06CH11357]; Argonne, a U.S. Department of Energy Office of Science laboratory [DE-AC02-06CH11357] FX This research was supported by the Office of Advanced Scientific Computing Research, Office of Science, U.S. Department of Energy, under contract DE-AC02-06CH11357. This manuscript has been created by UChicago Argonne, LLC, Operator of Argonne National Laboratory ("Argonne"). Argonne, a U.S. Department of Energy Office of Science laboratory, is operated under contract DE-AC02-06CH11357. The U.S. Government retains for itself, and others acting on its behalf, a paid-up nonexclusive, irrevocable worldwide license in said article to reproduce, prepare derivative works, distribute copies to the public, and perform publicly and display publicly, by or on behalf of the Government. NR 23 TC 3 Z9 3 U1 0 U2 0 PU SIAM PUBLICATIONS PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA SN 0895-4798 EI 1095-7162 J9 SIAM J MATRIX ANAL A JI SIAM J. Matrix Anal. Appl. PY 2015 VL 36 IS 1 BP 90 EP 109 DI 10.1137/13093426X PG 20 WC Mathematics, Applied SC Mathematics GA CF0HB UT WOS:000352222700005 ER PT S AU Gou, P Yepez-Martinez, T Szczepaniak, AP AF Gou, Peng Yepez-Martinez, Tochtli Szczepaniak, Adam P. BE Bijker, R Lerma, S Lizcano, D TI Coulomb gauge approach for charmonium meson and hybrid radiative transitions SO XXXVII SYMPOSIUM ON NUCLEAR PHYSICS SE Journal of Physics Conference Series LA English DT Proceedings Paper CT 37th Symposium on Nuclear Physics CY JAN 06-09, 2014 CL Cocoyoc, MEXICO ID MODEL; QCD; SPECTRUM AB We consider the lowest order interaction of the Foldy-Wouthuysen QED and QCD Hamiltonian in the Coulomb gauge approach, to describe radiative transitions between conventional and hybrids charmonium mesons. The results are compared to potential quark models and lattices calculations. C1 [Gou, Peng; Szczepaniak, Adam P.] Thomas Jefferson Natl Accelerator Facil, Newport News, VA 23606 USA. [Gou, Peng; Yepez-Martinez, Tochtli; Szczepaniak, Adam P.] Indiana Univ, Ctr Explorat Energy & Matter, Bloomington, IN 47408 USA. [Szczepaniak, Adam P.] Indiana Univ, Dept Phys, Bloomington, IN 47405 USA. RP Gou, P (reprint author), Thomas Jefferson Natl Accelerator Facil, Newport News, VA 23606 USA. EM pguo@jlab.org; tyepezma@indiana.edu; aszczepa@indiana.edu NR 35 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 2015 VL 578 AR 012016 DI 10.1088/1742-6596/578/1/012016 PG 6 WC Physics, Nuclear SC Physics GA BC3YM UT WOS:000352087300016 ER PT S AU Anselmino, M Boglione, M Gonzalez, JOH Melis, S Prokudin, A AF Anselmino, M. Boglione, M. Gonzalez, J. O. H. Melis, S. Prokudin, A. BE DAlesio, U Murgia, F TI Phenomenology of COMPASS data Multiplicities and Phenomenology - Part II SO 4TH INTERNATIONAL WORKSHOP ON TRANSVERSE POLARISATION PHENOMENA IN HARD PROCESSES (TRANSVERSITY 2014) SE EPJ Web of Conferences LA English DT Proceedings Paper CT 4th International Workshop on Transverse Polarisation Phenomena in Hard Processes (TRANSVERSITY) CY JUN 09-13, 2014 CL Cagliari, ITALY SP Italian Minist Educ AB present some of the main features of the multidimensional COMPASS multiplicities, via our analysis using the simple Gaussian model. We briefly discuss these results in connection with azimuthal asymmetries. C1 [Anselmino, M.; Boglione, M.; Melis, S.] Univ Turin, Dipartimento Fis Teor, I-10125 Turin, Italy. [Anselmino, M.; Boglione, M.; Gonzalez, J. O. H.] Ist Nazl Fis Nucl, Sez Torino, I-10125 Turin, Italy. [Prokudin, A.] Jefferson Lab, Newport News, VA 23606 USA. RP Anselmino, M (reprint author), Univ Turin, Dipartimento Fis Teor, Via P Giuria 1, I-10125 Turin, Italy. EM anselmino@to.infn.it; boglione@to.infn.it; joseosvaldo.gonzalez@to.infn.it; melis@to.infn.it; prokudin@jlab.gov OI Melis, Stefano/0000-0001-7316-4346; Boglione, Mariaelena/0000-0002-3647-1731; Anselmino, Mauro/0000-0003-0900-8001 NR 11 TC 0 Z9 0 U1 1 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 J9 EPJ WEB CONF PY 2015 VL 85 AR 02017 DI 10.1051/epjconf/20158502017 PG 5 WC Physics, Multidisciplinary SC Physics GA BC3PL UT WOS:000351841100026 ER PT S AU Avakian, H AF Avakian, Harut BE DAlesio, U Murgia, F TI Monte Carlo Generators for Studies of the 3D Structure of the Nucleon SO 4TH INTERNATIONAL WORKSHOP ON TRANSVERSE POLARISATION PHENOMENA IN HARD PROCESSES (TRANSVERSITY 2014) SE EPJ Web of Conferences LA English DT Proceedings Paper CT 4th International Workshop on Transverse Polarisation Phenomena in Hard Processes (TRANSVERSITY) CY JUN 09-13, 2014 CL Cagliari, ITALY SP Italian Minist Educ ID DEEP-INELASTIC SCATTERING; TRANSVERSE-MOMENTUM; PARTON DISTRIBUTIONS; QUARK; SPIN; ELECTROPRODUCTION; LEPTOPRODUCTION; FRAGMENTATION; QCD AB Extraction of transverse momentum and space distributions of partons from measurements of spin and azimuthal asymmetries requires development of a self consistent analysis framework, accounting for evolution effects, and allowing control of systematic uncertainties due to variations of input parameters and models. Development of realistic Monte-Carlo generators, accounting for TMD evolution effects, spin-orbit and quark-gluon correlations will be crucial for future studies of quark-gluon dynamics in general and 3D structure of the nucleon in particular. C1 Jefferson Lab, Newport News, VA 23606 USA. RP Avakian, H (reprint author), Jefferson Lab, 12000 Jefferson Ave, Newport News, VA 23606 USA. EM avakian@jlab.org NR 71 TC 1 Z9 1 U1 0 U2 1 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 J9 EPJ WEB CONF PY 2015 VL 85 AR 02023 DI 10.1051/epjconf/20158502023 PG 6 WC Physics, Multidisciplinary SC Physics GA BC3PL UT WOS:000351841100032 ER PT S AU Beppu, H Kanazawa, K Koike, Y Yoshida, S AF Beppu, Hiroo Kanazawa, Koichi Koike, Yuji Yoshida, Shinsuke BE DAlesio, U Murgia, F TI The role of three-gluon correlation functions in the single spin asymmetry SO 4TH INTERNATIONAL WORKSHOP ON TRANSVERSE POLARISATION PHENOMENA IN HARD PROCESSES (TRANSVERSITY 2014) SE EPJ Web of Conferences LA English DT Proceedings Paper CT 4th International Workshop on Transverse Polarisation Phenomena in Hard Processes (TRANSVERSITY) CY JUN 09-13, 2014 CL Cagliari, ITALY SP Italian Minist Educ ID DEEP-INELASTIC SCATTERING; HADRONIC PION-PRODUCTION; CHIRAL-ODD CONTRIBUTION; DIRECT-PHOTON; COLLISIONS AB We study the twist-3 three-gluon contribution to the single spin asymmetry in the light-hadron production in pp collision in the framework of the collinear factorization. We derive the corresponding cross section formula in the leading order with respect to the QCD coupling constant. We also present a numerical calculation of the asymmetry at the RHIC energy, using a model for the three-gluon correlation functions suggested by the asymmetry for the D-meson production at RHIC. We found that the asymmetries for the light-hadron and the jet productions are very useful to constrain the magnitude and form of the correlation functions. Since the three-gluon correlation functions shift the asymmetry for all kinds of hadrons in the same direction, it is unlikely that they become a main source of the asymmetry. C1 [Beppu, Hiroo; Kanazawa, Koichi] Niigata Univ, Grad Sch Sci & Technol, Niigata 9502181, Japan. [Kanazawa, Koichi] Temple Univ, Dept Phys, Philadelphia, PA 19122 USA. [Koike, Yuji] Niigata Univ, Dept Phys, Niigata 9502181, Japan. [Yoshida, Shinsuke] RIKEN, Nishina Ctr, Theoret Res Div, Wako, Saitama 3510198, Japan. [Yoshida, Shinsuke] Brookhaven Natl Lab, Dept Phys, Upton, NY 11973 USA. RP Beppu, H (reprint author), Niigata Univ, Grad Sch Sci & Technol, Niigata 9502181, Japan. EM beppu@nt.sc.niigata-u.ac.jp; koichi.kanazawa@temple.edu; koike@nt.sc.niigata-u.ac.jp; shinsuke.yoshida@riken.jp NR 38 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 J9 EPJ WEB CONF PY 2015 VL 85 AR 02012 DI 10.1051/epjconf/20158502012 PG 5 WC Physics, Multidisciplinary SC Physics GA BC3PL UT WOS:000351841100021 ER PT S AU Bland, LC AF Bland, L. C. BE DAlesio, U Murgia, F TI Transverse Single Spin Asymmetries in Hadronic Interactions An Experimental Overview and Outlook SO 4TH INTERNATIONAL WORKSHOP ON TRANSVERSE POLARISATION PHENOMENA IN HARD PROCESSES (TRANSVERSITY 2014) SE EPJ Web of Conferences LA English DT Proceedings Paper CT 4th International Workshop on Transverse Polarisation Phenomena in Hard Processes (TRANSVERSITY) CY JUN 09-13, 2014 CL Cagliari, ITALY SP Italian Minist Educ ID DEEP-INELASTIC SCATTERING; QUANTUM CHROMODYNAMICS; HARD-SCATTERING; ANALYZING POWER; POLARIZATION; MOMENTUM; PROTONS; JETS AB Transverse single-spin asymmetries (SSA) are expected to be small in perturbative QCD because of the chiral nature of the theory. Experiment shows there are large transverse SSA for particles produced in special kinematics. This contribution reviews the experimental situation and provides an outlook for future measurements. C1 Brookhaven Natl Lab, Upton, NY 11973 USA. RP Bland, LC (reprint author), Brookhaven Natl Lab, Upton, NY 11973 USA. NR 57 TC 0 Z9 0 U1 1 U2 1 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 J9 EPJ WEB CONF PY 2015 VL 85 AR 01008 DI 10.1051/epjconf/20158501008 PG 11 WC Physics, Multidisciplinary SC Physics GA BC3PL UT WOS:000351841100008 ER PT S AU Pitonyak, D Kanazawa, K Koike, Y Metz, A AF Pitonyak, Daniel Kanazawa, Koichi Koike, Yuji Metz, Andreas BE DAlesio, U Murgia, F TI A(N) in proton-proton collisions and the role of twist-3 fragmentation SO 4TH INTERNATIONAL WORKSHOP ON TRANSVERSE POLARISATION PHENOMENA IN HARD PROCESSES (TRANSVERSITY 2014) SE EPJ Web of Conferences LA English DT Proceedings Paper CT 4th International Workshop on Transverse Polarisation Phenomena in Hard Processes (TRANSVERSITY) CY JUN 09-13, 2014 CL Cagliari, ITALY SP Italian Minist Educ ID SINGLE-SPIN ASYMMETRY; PION-PRODUCTION; ANALYZING POWER; LEPTOPRODUCTION; DISTRIBUTIONS; POLARIZATION; SCATTERING; COLLINS; KAONS; BEAM AB We review and give an update on the current status of what causes transverse single-spin asymmetries (TSSAs) in semi-inclusive processes where a single hadron is detected in the final state, especially those involving proton-proton (pp) collisions. In particular, we provide a new analysis within collinear factorization of TSSAs in high transverse momentum charged and neutral pion production in pp collisions at the Relativistic Heavy Ion Collider (RHIC). This study incorporates the so-called twist-3 fragmentation term and shows that one can describe RHIC data through this mechanism. Moreover, by fixing other non-perturbative inputs through extractions of transverse momentum dependent functions in e(+)e(-) -> h(1)h(2)X and semi-inclusive deep-inelastic scattering (SIDIS), we provide for the first time a consistency between certain spin/azimuthal asymmetries in all three reactions (i.e., pp, e(+)e(-), and SIDIS). C1 [Pitonyak, Daniel] Brookhaven Natl Lab, RIKEN BNL Res Ctr, Upton, NY 11973 USA. [Kanazawa, Koichi] Niigata Univ, Grad Sch Sci & Technol, Niigata 9502181, Japan. [Kanazawa, Koichi; Metz, Andreas] Temple Univ, Dept Phys, Philadelphia, PA 19122 USA. [Koike, Yuji] Niigata Univ, Dept Phys, Niigata 9502181, Japan. RP Pitonyak, D (reprint author), Brookhaven Natl Lab, RIKEN BNL Res Ctr, Upton, NY 11973 USA. EM dpitonyak@quark.phy.bnl.gov; koichi.kanazawa@temple.edu; koike@nt.sc.niigata-u.ac.jp; metza@temple.edu NR 60 TC 0 Z9 0 U1 2 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 J9 EPJ WEB CONF PY 2015 VL 85 AR 02013 DI 10.1051/epjconf/20158502013 PG 6 WC Physics, Multidisciplinary SC Physics GA BC3PL UT WOS:000351841100022 ER PT S AU Prokudin, A AF Prokudin, Alexei BE DAlesio, U Murgia, F TI A(N) in inclusive lepton-proton collisions: TMD and twist-3 approaches SO 4TH INTERNATIONAL WORKSHOP ON TRANSVERSE POLARISATION PHENOMENA IN HARD PROCESSES (TRANSVERSITY 2014) SE EPJ Web of Conferences LA English DT Proceedings Paper CT 4th International Workshop on Transverse Polarisation Phenomena in Hard Processes (TRANSVERSITY) CY JUN 09-13, 2014 CL Cagliari, ITALY SP Italian Minist Educ ID SINGLE-SPIN ASYMMETRY; DEEP-INELASTIC SCATTERING; DIRECT PHOTON PRODUCTION; HARD-SCATTERING; PION-PRODUCTION; FRAGMENTATION; AZIMUTHAL; QCD AB We consider the inclusive production of hadrons in lepton-nucleon scattering. For a transversely polarized nucleon this reaction shows a left-right azimuthal asymmetry, which we compute in both TMD and in twist-3 collinear factorization formalisms. All non-perturbative parton correlators of the calculation are fixed through information from other hard processes. Our results for the left-right asymmetry agree in sign with recent data for charged pion production from the HERMES Collaboration and from Jefferson Lab. We discuss similarities and differences of the two formalisms. C1 Jefferson Lab, Newport News, VA 23606 USA. RP Prokudin, A (reprint author), Jefferson Lab, 12000 Jefferson Ave, Newport News, VA 23606 USA. EM prokudin@jlab.org NR 62 TC 0 Z9 0 U1 0 U2 1 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 J9 EPJ WEB CONF PY 2015 VL 85 AR 02028 DI 10.1051/epjconf/20158502028 PG 6 WC Physics, Multidisciplinary SC Physics GA BC3PL UT WOS:000351841100037 ER PT J AU Buchmann, LF Stamper-Kurn, DM AF Buchmann, Lukas F. Stamper-Kurn, Dan M. TI The quantum/classical transition in mediated interactions SO ANNALEN DER PHYSIK LA English DT Article DE Cavity optomechanics; quantum to classical transition; multimode optomechanics ID CAVITY OPTOMECHANICS; QUANTUM; ATOMS AB Two quantum modes interacting via local couplings to a dissipative bosonic field are investigated theoretically. The model considers two mechanical modes with distinct frequencies coupled optomechanically to the same cavity mode. The dissipative cavity field mediates the interaction between the mechanical modes but also leads to decoherence of the mechanical oscillators. Depending on the ratio between effective interaction strength and dissipation rate, which can be chosen via the pump detuning, the interaction assumes a quantum mechanical or classical character. The distinction between the two regimes is made by the ability of the mediated interaction to correlate the two mechanical modes non-classically. For any cavity decay, there is a regime where the two mechanical modes interact in a non-classical way, which leads us to conclude that optomechanical systems can serve as a model to experimentally study the transition of effective interactions mediated by classical or quantum-mechanical fields. C1 [Buchmann, Lukas F.; Stamper-Kurn, Dan M.] Univ Calif Berkeley, Dept Phys, Berkeley, CA 94720 USA. [Stamper-Kurn, Dan M.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. RP Buchmann, LF (reprint author), Univ Calif Berkeley, Dept Phys, Berkeley, CA 94720 USA. EM lbuchmann@berkeley.edu RI Stamper-Kurn, Dan/B-5442-2015; OI Stamper-Kurn, Dan/0000-0002-4845-5835; Buchmann, Lukas/0000-0002-2527-6789 FU SNSF; AFOSR; NSF FX This work was supported by the SNSF, AFOSR and NSF. LFB would like to thank D. Kafri and Y. Chen for useful discussions. NR 37 TC 6 Z9 6 U1 0 U2 4 PU WILEY-V C H VERLAG GMBH PI WEINHEIM PA POSTFACH 101161, 69451 WEINHEIM, GERMANY SN 0003-3804 EI 1521-3889 J9 ANN PHYS-BERLIN JI Ann. Phys.-Berlin PD JAN PY 2015 VL 527 IS 1-2 SI SI BP 156 EP 161 DI 10.1002/andp.201400150 PG 6 WC Physics, Multidisciplinary SC Physics GA CE2HC UT WOS:000351634800016 ER PT J AU Dickie, DA Ulibarri-Sanchez, RP Kemp, RA AF Dickie, Diane A. Ulibarri-Sanchez, Raymond P., III Kemp, Richard A. TI Zwitterionic CS2 Adducts of Bis(dialkylphosphino)amines: Syntheses, Spectroscopy, and Structures SO AUSTRALIAN JOURNAL OF CHEMISTRY LA English DT Article ID MOLECULAR-STRUCTURE; CARBON-DISULFIDE; CRYSTAL-STRUCTURES; DIOXIDE; COMPLEXES; TELLURIUM; LIGANDS; ION; CO2 AB Both bis(diisopropylphosphino)amine and bis(di-t-butylphosphino)amine react with CS2 to give bright red zwitterionic adducts of the form R2P(CS2)NP(R-2)H (R=Pr-i or Bu-t). The P-H tautomer is the exclusive species present in solution, and there is no evidence of CS2 lability. The tautomeric hydrogen can undergo exchange with deuterium in protic solvents such as CD3OD. The products were characterized by single-crystal X-ray diffraction, IR and multinuclear (H-1, H-2, C-13, P-31) NMR spectroscopies. C1 [Dickie, Diane A.; Kemp, Richard A.] Univ New Mexico, Dept Chem & Chem Biol, Albuquerque, NM 87131 USA. [Ulibarri-Sanchez, Raymond P., III; Kemp, Richard A.] Sandia Natl Labs, Adv Mat Lab, Albuquerque, NM 87106 USA. RP Kemp, RA (reprint author), Univ New Mexico, Dept Chem & Chem Biol, Albuquerque, NM 87131 USA. EM rakemp@unm.edu RI Dickie, Diane/B-1647-2010 OI Dickie, Diane/0000-0003-0939-3309 FU National Science Foundation [CHE12-13529]; Laboratory Directed Research and Development (LDRD) program at Sandia National Laboratories [LDRD 151300]; Sandia National Laboratories STAR student internship program; National Science Foundation CRIF:MU award [CHE04-43580]; NSF [CHE08-40523, CHE09-46690]; United States Department of Energy [DE-AC04-94AL85000] FX This work was financially supported by the National Science Foundation (grant CHE12-13529) and by the Laboratory Directed Research and Development (LDRD) program at Sandia National Laboratories (LDRD 151300) and the Sandia National Laboratories STAR student internship program. The Bruker X-ray diffractometer was purchased via a National Science Foundation CRIF:MU award to the University of New Mexico (CHE04-43580), and the NMR spectrometers were upgraded via grants from the NSF (CHE08-40523 and CHE09-46690). Sandia is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Co., for the United States Department of Energy under Contract No. DE-AC04-94AL85000. NR 30 TC 2 Z9 2 U1 0 U2 6 PU CSIRO PUBLISHING PI CLAYTON PA UNIPARK, BLDG 1, LEVEL 1, 195 WELLINGTON RD, LOCKED BAG 10, CLAYTON, VIC 3168, AUSTRALIA SN 0004-9425 EI 1445-0038 J9 AUST J CHEM JI Aust. J. Chem. PY 2015 VL 68 IS 3 BP 351 EP 356 DI 10.1071/CH14535 PG 6 WC Chemistry, Multidisciplinary SC Chemistry GA CE1DG UT WOS:000351551700002 ER PT J AU Visperas, PR Winger, JA Horton, TM Shah, NH Aum, DJ Tao, A Barros, T Yan, QR Wilson, CG Arkin, MR Weiss, A Kuriyan, J AF Visperas, Patrick R. Winger, Jonathan A. Horton, Timothy M. Shah, Neel H. Aum, Diane J. Tao, Alyssa Barros, Tiago Yan, Qingrong Wilson, Christopher G. Arkin, Michelle R. Weiss, Arthur Kuriyan, John TI Modification by covalent reaction or oxidation of cysteine residues in the tandem-SH2 domains of ZAP-70 and Syk can block phosphopeptide binding SO BIOCHEMICAL JOURNAL LA English DT Article DE B-cell; covalent small-molecule inhibitor; hydrogen peroxide (H2O2); immunoreceptor tyrosine-based activation motif (ITAM); T-cell ID T-CELL-RECEPTOR; TYROSINE KINASE ZAP-70; HYDROGEN-PEROXIDE; REDOX REGULATION; STRUCTURAL BASIS; SIGNAL-TRANSDUCTION; CRYSTAL-STRUCTURE; ANTIGEN RECEPTOR; SH2 INHIBITORS; IN-VIVO AB Zeta-chain associated protein of 70 kDa (ZAP-70) and spleen tyrosine kinase (Syk) are non-receptor tyrosine kinases that are essential for T-cell and B-cell antigen receptor signalling respectively. They are recruited, via their tandem-SH2 (Src-homology domain 2) domains, to doubly phosphorylated immunoreceptor tyrosine-based activation motifs (ITAMs) on invariant chains of immune antigen receptors. Because of their critical roles in immune signalling, ZAP-70 and Syk are targets for the development of drugs for autoimmune diseases. We show that three thiol-reactive small molecules can prevent the tandem-SH2 domains of ZAP-70 and Syk from binding to phosphorylated ITAMs. We identify a specific cysteine residue in the phosphotyrosine-binding pocket of each protein (Cys39 in ZAP-70, Cys206 in Syk) that is necessary for inhibition by two of these compounds. We also find that ITAMbinding to ZAP-70 and Syk is sensitive to the presence of H2O2 and these two cysteine residues are also necessary for inhibition by H2O2. Our findings suggest a mechanism by which the reactive oxygen species generated during responses to antigen could attenuate signalling through these kinases and may also inform the development of ZAP-70 and Syk inhibitors that bind covalently to their SH2 domains. C1 [Visperas, Patrick R.; Winger, Jonathan A.; Horton, Timothy M.; Shah, Neel H.; Aum, Diane J.; Tao, Alyssa; Barros, Tiago; Yan, Qingrong; Kuriyan, John] Univ Calif Berkeley, Calif Inst Quantitat Biosci, Dept Mol & Cell Biol, Berkeley, CA 94720 USA. [Visperas, Patrick R.; Winger, Jonathan A.; Horton, Timothy M.; Shah, Neel H.; Aum, Diane J.; Tao, Alyssa; Barros, Tiago; Yan, Qingrong; Kuriyan, John] Univ Calif Berkeley, Calif Inst Quantitat Biosci, Dept Chem, Berkeley, CA 94720 USA. [Visperas, Patrick R.; Winger, Jonathan A.; Horton, Timothy M.; Shah, Neel H.; Aum, Diane J.; Tao, Alyssa; Barros, Tiago; Yan, Qingrong; Kuriyan, John] Univ Calif Berkeley, Howard Hughes Med Inst, Berkeley, CA 94720 USA. [Wilson, Christopher G.; Arkin, Michelle R.] Univ Calif San Francisco, Small Mol Discovery Ctr, Dept Pharmaceut Chem, San Francisco, CA 94158 USA. [Weiss, Arthur] Univ Calif San Francisco, Rosalind Russell & Ephrain P Engleman Rheumatol R, Dept Med, San Francisco, CA 94143 USA. [Weiss, Arthur] Univ Calif San Francisco, Howard Hughes Med Inst, San Francisco, CA 94143 USA. [Kuriyan, John] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 USA. RP Kuriyan, J (reprint author), Univ Calif Berkeley, Calif Inst Quantitat Biosci, Dept Mol & Cell Biol, Berkeley, CA 94720 USA. EM kuriyan@berkeley.edu RI Winger, Jonathan/B-3885-2010; OI Barros, Tiago/0000-0002-9807-7625; Winger, Jonathan/0000-0003-1413-3384; Shah, Neel H/0000-0002-1186-0626 FU National Institute of Arthritis and Musculoskeletal and Skin Diseases/National Institutes of Health American Recovery and Reinvest Act [1RC2-AR058947-01]; National Institutes of Health/National Cancer Institute UC Berkeley Cancer Laboratory training grant [5T32 CA 9179-35] FX This work was supported by the National Institute of Arthritis and Musculoskeletal and Skin Diseases/National Institutes of Health American Recovery and Reinvest Act [grant number 1RC2-AR058947-01 (to A.W. and J.K.)] and the National Institutes of Health/National Cancer Institute UC Berkeley Cancer Laboratory training grant [grant number 5T32 CA 9179-35 (to P.R.V.)]. NR 42 TC 4 Z9 4 U1 0 U2 14 PU PORTLAND PRESS LTD PI LONDON PA CHARLES DARWIN HOUSE, 12 ROGER STREET, LONDON WC1N 2JU, ENGLAND SN 0264-6021 EI 1470-8728 J9 BIOCHEM J JI Biochem. J. PD JAN 1 PY 2015 VL 465 BP 149 EP 161 DI 10.1042/BJ20140793 PN 1 PG 13 WC Biochemistry & Molecular Biology SC Biochemistry & Molecular Biology GA CE2XN UT WOS:000351685300012 PM 25287889 ER PT J AU Heistermann, M Collis, S Dixon, MJ Giangrande, S Helmus, JJ Kelley, B Koistinen, J Michelson, DB Peura, M Pfaff, T Wolff, DB AF Heistermann, M. Collis, S. Dixon, M. J. Giangrande, S. Helmus, J. J. Kelley, B. Koistinen, J. Michelson, D. B. Peura, M. Pfaff, T. Wolff, D. B. TI THE EMERGENCE OF OPEN-SOURCE SOFTWARE FOR THE WEATHER RADAR COMMUNITY SO BULLETIN OF THE AMERICAN METEOROLOGICAL SOCIETY LA English DT Article ID C-BAND RADAR; REAL-TIME; ATTENUATION CORRECTION; RAINFALL ESTIMATION; DIFFERENTIAL PHASE; MOUNTAINOUS REGION; BEAM BLOCKAGE; IDENTIFICATION; ALGORITHMS; RETRIEVAL AB Weather radar analysis has become increasingly sophisticated over the past 50 years, and efforts to keep software up to date have generally lagged behind the needs of the users. We argue that progress has been impeded by the fact that software has not been developed and shared as a community. Recently, the situation has been changing. In this paper, the developers of a number of open-source software (OSS) projects highlight the potential of OSS to advance radar-related research. We argue that the community-based development of OSS holds the potential to reduce duplication of efforts and to create transparency in implemented algorithms while improving the quality and scope of the software. We also conclude that there is sufficiently mature technology to support collaboration across different software projects. This could allow for consolidation toward a set of interoperable software platforms, each designed to accommodate very specific user requirements. C1 [Heistermann, M.] Univ Potsdam, Inst Earth & Environm Sci, D-14476 Potsdam, Germany. [Collis, S.; Helmus, J. J.] Argonne Natl Lab, Argonne, IL 60439 USA. [Dixon, M. J.] Natl Ctr Atmospher Res, Boulder, CO 80307 USA. [Giangrande, S.] Brookhaven Natl Lab, Biol Environm & Climate Sci Dept, Upton, NY 11973 USA. [Kelley, B.; Wolff, D. B.] NASA, Goddard Space Flight Ctr, Wallops Flight Facil, Wallops Isl, VA 23337 USA. [Koistinen, J.; Peura, M.] Finnish Meteorol Inst, FIN-00101 Helsinki, Finland. [Michelson, D. B.] Swedish Meteorol & Hydrol Inst, S-60176 Norrkoping, Sweden. [Pfaff, T.] Univ Stuttgart, Inst Wasser & Umweltsyst Modellie, D-70174 Stuttgart, Germany. RP Heistermann, M (reprint author), Univ Potsdam, Karl Liebknecht Str 24-25, D-14476 Potsdam, Germany. EM maik.heistermann@uni-potsdam.de RI Giangrande, Scott/I-4089-2016 OI Giangrande, Scott/0000-0002-8119-8199 FU U.S. Federal Aviation Administration; U.S. National Science Foundation; European Union (European Regional Development Fund); European Union (European Neighbourhood and Partnership Instrument); U.S. Department of Energy, Office of Science, Office of Biological and Environmental Research [DE-AC02-06CH11357]; Office of Biological and Environmental Research (OBER) of the U.S. Department of Energy (DOE) as part of ARM; German Federal Ministry for Research and Education within the PROGRESS project; NASA's Precipitation Measurement Missions program FX The development of TITAN was funded by the U.S. Federal Aviation Administration. The development of LROSE is funded by the U.S. National Science Foundation. BALTRAD software has been developed as part of the BALTRAD and BALTRAD+ projects that have been partly financed by the European Union (European Regional Development Fund and European Neighbourhood and Partnership Instrument). Argonne National Laboratory's work was supported by the U.S. Department of Energy, Office of Science, Office of Biological and Environmental Research, under Contract DE-AC02-06CH11357. This work has been supported by the Office of Biological and Environmental Research (OBER) of the U.S. Department of Energy (DOE) as part of ARM. The development of wradlib was partly funded by the German Federal Ministry for Research and Education within the PROGRESS project, The development of RSL and RSL-in-IDL were supported by NASA's Precipitation Measurement Missions program. The authors thank Jonathan J. Gourley, Norman Donaldson, and Marco Borga who reviewed this paper and who substantially contributed to its improvement. NR 51 TC 7 Z9 7 U1 0 U2 6 PU AMER METEOROLOGICAL SOC PI BOSTON PA 45 BEACON ST, BOSTON, MA 02108-3693 USA SN 0003-0007 EI 1520-0477 J9 B AM METEOROL SOC JI Bull. Amer. Meteorol. Soc. PD JAN PY 2015 VL 96 IS 1 BP 117 EP 128 DI 10.1175/BAMS-D-13-00240.1 PG 12 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA CE0FA UT WOS:000351478700016 ER PT J AU Wu, QY Xiong, SM Shen, PC Zhao, S Li, Y Su, D Orlov, A AF Wu, Qiyuan Xiong, Shangmin Shen, Peichuan Zhao, Shen Li, Yan Su, Dong Orlov, Alexander TI Exceptional activity of sub-nm Pt clusters on CdS for photocatalytic hydrogen production: a combined experimental and first-principles study SO CATALYSIS SCIENCE & TECHNOLOGY LA English DT Article ID HIGH QUANTUM EFFICIENCY; VISIBLE-LIGHT; H-2-PRODUCTION PERFORMANCE; NOBLE-METAL; FUEL-CELLS; PT-PDS/CDS; WATER; GENERATION; EVOLUTION; CATALYSTS C1 [Wu, Qiyuan; Xiong, Shangmin; Shen, Peichuan; Zhao, Shen; Li, Yan; Su, Dong; Orlov, Alexander] SUNY Stony Brook, Dept Mat Sci & Engn, Stony Brook, NY 11794 USA. [Li, Yan] Brookhaven Natl Lab, Computat Sci Ctr, Upton, NY 11973 USA. [Su, Dong] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. RP Orlov, A (reprint author), SUNY Stony Brook, Dept Mat Sci & Engn, Stony Brook, NY 11794 USA. EM alexander.orlov@stonybrook.edu RI Su, Dong/A-8233-2013 OI Su, Dong/0000-0002-1921-6683 FU NSF DMR award [1231586]; U.S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10086]; Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231] FX Alexander Orlov would like to acknowledge financial support from the NSF DMR award #1231586. Work performed by Shangmin Xiong, Yan Li and Dong Su was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, under contract no. DE-AC02-98CH10086. TEM measurements and DFT calculations were carried out at the Center for Functional Nanomaterials at Brookhaven National Laboratory, which is supported by the U.S. Department of Energy, Office of Basic Energy Sciences, under contract no. DE-AC02-98CH10886. This research also used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under contract no. DE-AC02-05CH11231. We would also like to thank Dr. Mike White for his help in the XPS experiment. NR 36 TC 3 Z9 3 U1 2 U2 27 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2044-4753 EI 2044-4761 J9 CATAL SCI TECHNOL JI Catal. Sci. Technol. PY 2015 VL 5 IS 4 BP 2059 EP 2064 DI 10.1039/c4cy01563k PG 6 WC Chemistry, Physical SC Chemistry GA CE3QH UT WOS:000351742700005 ER PT J AU Lu, HF Zhang, PF Qiao, ZA Zhang, JS Zhu, HY Chen, JH Chen, YF Dai, S AF Lu, Hanfeng Zhang, Pengfei Qiao, Zhen-An Zhang, Jinshui Zhu, Huiyuan Chen, Jihua Chen, Yinfei Dai, Sheng TI Ionic liquid-mediated synthesis of meso-scale porous lanthanum-transition-metal perovskites with high CO oxidation performance SO CHEMICAL COMMUNICATIONS LA English DT Article ID OXYGEN REDUCTION CATALYSTS; HIGH-SURFACE-AREA; STRUCTURAL STABILITY; MESOPOROUS SILICA; LACOO3 PEROVSKITE; COMBUSTION; NANOPARTICLES; TEMPLATE; CARBON; LAMNO3 AB Lanthanum-transition-metal perovskites with robust meso-scale porous frameworks (meso-LaMO3) are synthesized through the use of ionic liquids. The resultant samples demonstrate a rather high activity for CO oxidation, by taking advantage of unique nanostructure-derived benefits. This synthesis strategy opens up a new opportunity for preparing functional mesoporous complex oxides of various compositions. C1 [Lu, Hanfeng; Chen, Yinfei] Zhejiang Univ Technol, Inst Catalyt React Engn, Coll Chem Engn, Hangzhou 310014, Zhejiang, Peoples R China. [Lu, Hanfeng; Zhang, Pengfei; Qiao, Zhen-An; Zhang, Jinshui; Zhu, Huiyuan; Dai, Sheng] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN 37831 USA. [Chen, Jihua] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN USA. [Chen, Jihua] Oak Ridge Natl Lab, Div Chem Sci, Oak Ridge, TN USA. [Dai, Sheng] Univ Tennessee, Dept Chem, Knoxville, TN 37996 USA. RP Lu, HF (reprint author), Zhejiang Univ Technol, Inst Catalyt React Engn, Coll Chem Engn, Hangzhou 310014, Zhejiang, Peoples R China. EM luhf@zjut.edu.cn; dais@ornl.gov RI Chen, Jihua/F-1417-2011; Lu, Hanfeng/D-1017-2014; Dai, Sheng/K-8411-2015; Zhang, Pengfei/I-5484-2013; zhang, Jinshui/D-9749-2016; OI Chen, Jihua/0000-0001-6879-5936; Dai, Sheng/0000-0002-8046-3931; zhang, Jinshui/0000-0003-4649-6526; Qiao, Zhen-An/0000-0001-6064-9360 FU U.S. Department of Energy, Office of Science, Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division; Natural Science Foundation of China [21107096]; Natural Science Foundation of Zhejiang province [LY14E080008]; Commission of Science and Technology of Zhejiang province [2013C03021] FX This work was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, the Natural Science Foundation of China (No. 21107096). HL and YC were supported in part by the Natural Science Foundation of Zhejiang province (No. LY14E080008) and the Commission of Science and Technology of Zhejiang province (No. 2013C03021). NR 47 TC 8 Z9 8 U1 16 U2 123 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1359-7345 EI 1364-548X J9 CHEM COMMUN JI Chem. Commun. PY 2015 VL 51 IS 27 BP 5910 EP 5913 DI 10.1039/c5cc00534e PG 4 WC Chemistry, Multidisciplinary SC Chemistry GA CE2QN UT WOS:000351660500024 PM 25727232 ER PT J AU Chen, XY Li, H Yin, PC Liu, TB AF Chen, Xinyue Li, Hui Yin, Panchao Liu, Tianbo TI Design of polystyrene latex particles covered with polyoxometalate clusters via multiple covalent bonding SO CHEMICAL COMMUNICATIONS LA English DT Article ID GOLD NANOPARTICLES; TRANSITION-METAL; ORGANIC HYBRID; OXIDATION; CATALYSTS; WATER; SURFACTANTS; REACTIVITY; NANOSCALE; MONOLAYER AB Polyoxometalates (POMs) covalently functionalized with methyl methacrylate groups were applied as surfactants in the emulsion polymerization reaction of styrene. Due to the copolymerization of the methyl methacrylate groups and the styrene monomers, the polyoxometalate clusters are covalently grafted onto the surface of polystyrene latex nanoparticles. Such latex particles are fully covered with catalytic POM clusters and might serve as quasi-homogeneous catalysts. C1 [Chen, Xinyue; Li, Hui; Yin, Panchao; Liu, Tianbo] Univ Akron, Dept Polymer Sci, Akron, OH 44325 USA. [Yin, Panchao] Oak Ridge Natl Lab, Neutron Sci Directorate, Chem & Engn Mat Div, Oak Ridge, TN 37831 USA. RP Yin, PC (reprint author), Univ Akron, Dept Polymer Sci, Akron, OH 44325 USA. EM yinp@ornl.gov; pyin@uakron.edu; tliu@uakron.edu RI Yin, Panchao/J-3322-2013; Liu, Tianbo/D-8915-2017 OI Yin, Panchao/0000-0003-2902-8376; Liu, Tianbo/0000-0002-8181-1790 FU NSF [CHE1305756]; University of Akron; Neutron Science Directorate in Oak Ridge National Laboratory; Office of Science of the US Department of Energy [DE-AC05-00OR22725] FX This work was supported by NSF (CHE1305756) and the University of Akron. Panchao Yin acknowledges the Clifford G. Shull Fellowship support from Neutron Science Directorate in Oak Ridge National Laboratory, which is supported by the Office of Science of the US Department of Energy under Contract No. DE-AC05-00OR22725. NR 40 TC 3 Z9 4 U1 6 U2 29 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1359-7345 EI 1364-548X J9 CHEM COMMUN JI Chem. Commun. PY 2015 VL 51 IS 28 BP 6104 EP 6107 DI 10.1039/c5cc00239g PG 4 WC Chemistry, Multidisciplinary SC Chemistry GA CE4YL UT WOS:000351836300010 PM 25743436 ER PT J AU Weiss, CJ Wiedner, ES Roberts, JAS Appel, AM AF Weiss, Charles J. Wiedner, Eric S. Roberts, John A. S. Appel, Aaron M. TI Nickel phosphine catalysts with pendant amines for electrocatalytic oxidation of alcohols SO CHEMICAL COMMUNICATIONS LA English DT Article ID CARBON; ENERGY; ELECTROOXIDATION; ACETONITRILE; REDUCTION; COMPLEXES; CHEMICALS; EFFICIENT; BASICITY; STORAGE AB Nickel phosphine complexes with pendant amines have been found to be electrocatalysts for the oxidation of primary and secondary alcohols, with turnover frequencies as high as 3.3 s(-1). These complexes are the first electrocatalysts for alcohol oxidation based on non-precious metals, which will be critical for use in fuel cells. C1 [Weiss, Charles J.; Wiedner, Eric S.; Roberts, John A. S.; Appel, Aaron M.] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Appel, AM (reprint author), Pacific NW Natl Lab, POB 999,MS K2-57, Richland, WA 99352 USA. EM aaron.appel@pnnl.gov OI Wiedner, Eric/0000-0002-7202-9676; Appel, Aaron/0000-0002-5604-1253 FU U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences Bio-sciences; Center for Molecular Electrocatalysis, Energy Frontier Research Center - U.S. Department of Energy, Office of Science FX The research by CJW, ESW, and AMA was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences & Bio-sciences. The research by JASR was supported as part of the Center for Molecular Electrocatalysis, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science. Pacific Northwest National Laboratory is operated by Battelle for the U.S. Department of Energy. NR 25 TC 14 Z9 14 U1 3 U2 17 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1359-7345 EI 1364-548X J9 CHEM COMMUN JI Chem. Commun. PY 2015 VL 51 IS 28 BP 6172 EP 6174 DI 10.1039/c5cc01107h PG 3 WC Chemistry, Multidisciplinary SC Chemistry GA CE4YL UT WOS:000351836300028 PM 25753760 ER PT J AU Pan, BF Zhang, JJ Huang, JH Vaughey, JT Zhang, L Han, SD Burrell, AK Zhang, ZC Liao, C AF Pan, Baofei Zhang, Junjie Huang, Jinhua Vaughey, John T. Zhang, Lu Han, Sang-Don Burrell, Anthony K. Zhang, Zhengcheng Liao, Chen TI A Lewis acid-free and phenolate-based magnesium electrolyte for rechargeable magnesium batteries SO CHEMICAL COMMUNICATIONS LA English DT Article ID ARYLOXIDES; STABILITY; CATHODE; SALTS AB A novel Lewis acid-free and phenolate-based magnesium electrolyte has been established. The excellent reversibility and stability of this electrolyte in battery cycling render this novel Lewis acid-free synthetic approach as a highly promising alternative for the development of highly anodically stable magnesium electrolytes for rechargeable magnesium batteries. C1 [Pan, Baofei; Huang, Jinhua; Vaughey, John T.; Zhang, Lu; Han, Sang-Don; Burrell, Anthony K.; Zhang, Zhengcheng; Liao, Chen] Argonne Natl Lab, Joint Ctr Energy Storage Res, Lemont, IL 60439 USA. [Pan, Baofei; Huang, Jinhua; Vaughey, John T.; Zhang, Lu; Han, Sang-Don; Burrell, Anthony K.; Zhang, Zhengcheng; Liao, Chen] Argonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USA. [Zhang, Junjie] Argonne Natl Lab, Div Mat Sci, Lemont, IL 60439 USA. RP Liao, C (reprint author), Argonne Natl Lab, Joint Ctr Energy Storage Res, 9700 S Cass Ave, Lemont, IL 60439 USA. EM liaoc@anl.gov RI Pan, Baofei/H-2867-2015; Zhang, junjie/C-4129-2008; OI Zhang, junjie/0000-0002-5561-1330; Liao, Chen/0000-0001-5168-6493; Vaughey, John/0000-0002-2556-6129 FU Joint Center for Energy Storage Research, an Energy Innovation Hub - U.S. Department of Energy, Office of Science, Basic Energy Sciences; U.S. Department of Energy Office of Science laboratory [DE-AC02-06CH11357] FX This work was supported as part of the Joint Center for Energy Storage Research, an Energy Innovation Hub funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences. 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. NR 20 TC 12 Z9 12 U1 5 U2 71 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1359-7345 EI 1364-548X J9 CHEM COMMUN JI Chem. Commun. PY 2015 VL 51 IS 28 BP 6214 EP 6217 DI 10.1039/c5cc01225b PG 4 WC Chemistry, Multidisciplinary SC Chemistry GA CE4YL UT WOS:000351836300039 PM 25758092 ER PT J AU Subbarao, U Jana, R Chondroudi, M Balasubramanian, M Kanatzidis, MG Peter, SC AF Subbarao, Udumula Jana, Rajkumar Chondroudi, Maria Balasubramanian, Mahalingam Kanatzidis, Mercouri G. Peter, Sebastian C. TI Yb7Ni4InGe12: a quaternary compound having mixed valent Yb atoms grown from indium flux SO DALTON TRANSACTIONS LA English DT Article ID X-RAY ABSORPTION; CRYSTAL-STRUCTURE; LIQUID INDIUM; EXPLORATORY SYNTHESIS; METAL FLUX; INTERMETALLIC COMPOUNDS; ORDERED SUPERSTRUCTURE; NEUTRON-DIFFRACTION; ALUMINUM SILICIDES; TERNARY SILICIDES AB The new intermetallic compound Yb7Ni4InGe12 was obtained as large silver needle shaped single crystals from reactive indium flux. Single crystal X-ray diffraction suggests that Yb7Ni4InGe12 crystallizes in the Yb7Ni4InGe12 structure type, and tetragonal space group P4/m and lattice constants are a = b = 10.291(2) angstrom and c = 4.1460(8)angstrom. The crystal structure of Yb7Ni4InGe12 consists of columnar units of three different types of channels filled with the Yb atoms. The crystal structure of Yb7Ni4InGe12 is closely related to Yb5Ni4Ge10. The effective magnetic moment obtained from the magnetic susceptibility measurements in the temperature range 200-300 K is 3.66 mu(B)/Yb suggests mixed/intermediate valence behavior of ytterbium atoms. X-ray absorption near edge spectroscopy (XANES) confirms that Yb7Ni4InGe12 exhibits mixed valence. C1 [Subbarao, Udumula; Jana, Rajkumar; Peter, Sebastian C.] Jawaharlal Nehru Ctr Adv Sci Res, New Chem Unit, Bangalore 560064, Karnataka, India. [Chondroudi, Maria; Kanatzidis, Mercouri G.] Argonne Natl Lab, Div Mat Sci, Argonne, IL 60439 USA. [Balasubramanian, Mahalingam] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. [Kanatzidis, Mercouri G.] Northwestern Univ, Dept Chem, Evanston, IL 60208 USA. RP Peter, SC (reprint author), Jawaharlal Nehru Ctr Adv Sci Res, New Chem Unit, Bangalore 560064, Karnataka, India. EM m-kanatzidis@northwestern.edu; sebastiancp@jncasr.ac.in FU Jawaharlal Nehru Centre for Advanced Scientific Research, Sheikh Saqr Laboratory and Department of Science and Technology (DST), India; JNCASR; DST [SR/S2/RJN-24/2010]; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]; U.S. Department of Energy (DOE) FX We thank Jawaharlal Nehru Centre for Advanced Scientific Research, Sheikh Saqr Laboratory and Department of Science and Technology (DST), India for the financial support. U.S. thanks CSIR and R. J thanks JNCASR and DST for research fellowship. S. C. P thanks DST for the Ramanujan fellowship (Grant SR/S2/RJN-24/2010). Research at Argonne National Laboratory is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract no. DE-AC02-06CH11357. We thank Prof. C. N. R. Rao for his constant support and encouragement. XSD/PNC facilities and research at these facilities are supported by the U.S. Department of Energy (DOE) and its founding institutions. NR 82 TC 3 Z9 3 U1 4 U2 12 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1477-9226 EI 1477-9234 J9 DALTON T JI Dalton Trans. PY 2015 VL 44 IS 12 BP 5797 EP 5804 DI 10.1039/c4dt03783a PG 8 WC Chemistry, Inorganic & Nuclear SC Chemistry GA CD9SS UT WOS:000351439200057 PM 25714934 ER PT J AU Ansari, SA Mohapatra, PK Verboom, W Zhang, ZC Dau, PD Gibson, JK Rao, LF AF Ansari, Seraj A. Mohapatra, Prasanta K. Verboom, Willem Zhang, Zhicheng Dau, Phuong D. Gibson, John K. Rao, Linfeng TI Binding of pyrazine-functionalized calix[4]arene ligands with lanthanides in an ionic liquid: thermodynamics and coordination modes SO DALTON TRANSACTIONS LA English DT Article ID F-ELEMENTS; PHOSPHORUS PRONUCLEOPHILES; EQUILIBRIUM-CONSTANTS; UNUSUAL COMPLEXATION; EXTRACTION; DIGLYCOLAMIDES; ACTINIDE; EUROPIUM; LUMINESCENCE; RECOGNITION AB The complexation of representative lanthanides with three calix[4]arenes functionalized with four pyrazine pendent arms containing different substituents such as carbamoyl dioctyl (L-I), diisopropyl phosphonate (L-II), and diphenyl phosphoryl (L-III) was investigated in water-saturated 1-butyl-3-methylimidazolium bis(trifluoromethanesulfonyl)imide (BumimTf(2)N) by absorption spectroscopy, luminescence spectroscopy, and microcalorimetry. All three ligands form 1 : 1 ML complexes (M = Eu3+ and L = ligand), and the stability constants (log beta) follow the order: L-I (-1.38 +/- 0.66) << L-II (3.71 +/- 0.02) < L-III (7.47 +/- 0.03), similar to the trend in the metal distribution coefficients in solvent extraction using these ligands as extractants. The enthalpy of complexation, determined by microcalorimetry, shows that the complexation of lanthanides with these bulky ligands is exothermic, and proceeds via replacement of water molecules from the primary coordination spheres. The 1 : 1 stoichiometry of the ML complexes was confirmed by electrospray ionization mass spectrometry. Results from optical absorption, luminescence and P-31-NMR spectroscopy suggest that, out of four pendent arms on the rigid calixarene platform, only two arms coordinate with the lanthanide ion and each arm is tridentate. The influence of structural features of the ligand on the complexation of lanthanides is explained with the help of thermodynamic parameters. C1 [Ansari, Seraj A.; Zhang, Zhicheng; Dau, Phuong D.; Gibson, John K.; Rao, Linfeng] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. [Ansari, Seraj A.; Mohapatra, Prasanta K.] Bhabha Atom Res Ctr, Div Radiochem, Bombay 400085, Maharashtra, India. [Verboom, Willem] Univ Twente, Inst Nanotechnol, Lab Mol Nanofabricat, NL-7500 AE Enschede, Netherlands. RP Rao, LF (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. EM LRao@lbl.gov FU Office of Science, Office of Basic Energy Science of the U.S. Department of Energy (DOE) at LBNL [DE-AC02-05CH11231]; Indo-US Science & Technology Forum (IUSSTF) FX This work was supported by the Director, Office of Science, Office of Basic Energy Science of the U.S. Department of Energy (DOE), under contract no. DE-AC02-05CH11231 at LBNL. SAA acknowledges the Indo-US Science & Technology Forum (IUSSTF) for awarding a fellowship. NR 24 TC 4 Z9 4 U1 6 U2 40 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1477-9226 EI 1477-9234 J9 DALTON T JI Dalton Trans. PY 2015 VL 44 IS 14 BP 6416 EP 6422 DI 10.1039/c5dt00049a PG 7 WC Chemistry, Inorganic & Nuclear SC Chemistry GA CE3QT UT WOS:000351744000015 PM 25747665 ER PT S AU Pratt, ST Jungen, C AF Pratt, S. T. Jungen, Ch. BE Schneider, IF Dulieu, O Robert, J TI General features of the dissociative recombination of polyatomic molecules SO DR2013: NINTH INTERNATIONAL CONFERENCE ON DISSOCIATIVE RECOMBINATION: THEORY, EXPERIMENT, AND APPLICATIONS SE EPJ Web of Conferences LA English DT Proceedings Paper CT 9th International Conference on Dissociative Recombination: Theory, Experiment, and Applications CY JUL 07-12, 2013 CL Paris, FRANCE AB We discuss some aspects of a simple expression for the low-energy dissociative recombination cross section that applies when the recombination process is dominated by the indirect mechanism. In most previous applications, this expression has been applied to capture into vibrationally excited Rydberg states with the assumption that capture is always followed by prompt dissociation. Here we consider the dissociative recombination of larger polyatomic ions and electrons. More specifically, we consider capture into electronically core-excited Rydberg states, and begin to assess its potential importance for larger systems. C1 [Pratt, S. T.] Argonne Natl Lab, Argonne, IL 60439 USA. [Jungen, Ch.] Univ Paris 11, Lab Aime Cotton CNRS, F-91405 Orsay, France. [Jungen, Ch.] UCL, Dept Phys & Astron, London WC1E 6BT, England. RP Pratt, ST (reprint author), Argonne Natl Lab, Bldg 200, Argonne, IL 60439 USA. EM stpratt@anl.gov NR 25 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 J9 EPJ WEB CONF PY 2015 VL 84 AR 04001 DI 10.1051/epjconf/20158404001 PG 5 WC Chemistry, Physical; Physics, Multidisciplinary SC Chemistry; Physics GA BC3PG UT WOS:000351835100012 ER PT J AU Mason, CW Lange, F Saravanan, K Lin, F Nordlund, D AF Mason, Chad W. Lange, Felix Saravanan, Kuppan Lin, Feng Nordlund, Dennis TI Beyond Divalent Copper: A Redox Couple for Sodium Ion Battery Cathode Materials SO ECS ELECTROCHEMISTRY LETTERS LA English DT Article ID RAY-ABSORPTION-SPECTROSCOPY; LI-ION; ELECTRODE; ALPHA-NAFEO2; P2-TYPE; OXIDES AB A P2-layered oxide using copper as the active redox metal has been discovered. It has a composition of Na2/3Cu1/3Mn2/3O2, and can withstand a thousand cycles, maintaining 61% of its original capacity. We demonstrate that copper can enable not only high voltage, but also excellent stability. This work opens up a new avenue of oxide design for high energy, cost effective battery systems. (C) The Author(s) 2015. Published by ECS. C1 [Mason, Chad W.; Lange, Felix] TUM CREATE, Singapore 138602, Singapore. [Saravanan, Kuppan; Lin, Feng] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. [Nordlund, Dennis] SLAC Natl Accelerator Lab, Stanford Synchrotron Radiat Lightsource, Menlo Pk, CA 94025 USA. RP Mason, CW (reprint author), TUM CREATE, Singapore 138602, Singapore. EM chadwmason@gmail.com RI Nordlund, Dennis/A-8902-2008 OI Nordlund, Dennis/0000-0001-9524-6908 FU Singapore National Research Foundation (NRF) through Campus for Research Excellence and Technological Enterprise (CREATE) program; Stanford Synchrotron Radiation Lightsource, Directorate of SLAC National Accelerator Laboratory; U.S. Department of Energy Office of Science FX The present work was supported by the Singapore National Research Foundation (NRF) through its Campus for Research Excellence and Technological Enterprise (CREATE) program. The authors acknowledge the support of Stanford Synchrotron Radiation Lightsource, a Directorate of SLAC National Accelerator Laboratory and an Office of Science User Facility operated for the U.S. Department of Energy Office of Science by Stanford University. Guidance and support from Dr. Guoying Chen and Dr. Marca Doeff at LBNL is greatly appreciated. We thank Arun Nagasubramanian, Steffen Schluter, Shahnaz Ghasemi, Heryani Ahmad, Irina Gocheva, and Denis Yu for discussions and support. We also thank Dr. Ryan Davis for assisting with the synchrotron experiments. NR 30 TC 0 Z9 0 U1 5 U2 34 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 2162-8726 EI 2162-8734 J9 ECS ELECTROCHEM LETT JI ECS Electrochem. Lett. PY 2015 VL 4 IS 5 BP A1 EP A4 DI 10.1149/2.0041505ee1 PG 4 WC Electrochemistry; Materials Science, Multidisciplinary SC Electrochemistry; Materials Science GA CE3CJ UT WOS:000351701600001 ER PT B AU Edelstein, FS AF Edelstein, Frederick S. BE Cooper, BS Cibulka, JG Fusarelli, LD TI ADVOCATES AND PARTNERS FOR EDUCATION EXCELLENCE A 21st-Century Role for Mayors SO HANDBOOK OF EDUCATION POLITICS AND POLICY, 2ND EDITION LA English DT Article; Book Chapter C1 [Edelstein, Frederick S.] US DOE, Washington, DC 20585 USA. NR 39 TC 0 Z9 0 U1 0 U2 0 PU ROUTLEDGE PI ABINGDON PA 2 PARK SQ, MILTON PARK, ABINGDON OX14 4RN, OXFORD, ENGLAND BN 978-0-415-66044-0; 978-0-203-07410-7; 978-0-415-66042-6 PY 2015 BP 62 EP 85 PG 24 WC Education & Educational Research; Public Administration SC Education & Educational Research; Public Administration GA BB9SS UT WOS:000348597900004 ER PT J AU Duan, S Peisert, S Levitt, KN AF Duan, Sisi Peisert, Sean Levitt, Karl N. TI hBFT: Speculative Byzantine Fault Tolerance with Minimum Cost SO IEEE TRANSACTIONS ON DEPENDABLE AND SECURE COMPUTING LA English DT Article DE Distributed systems; client/server; fault tolerance; state machine replication ID ASYNCHRONOUS CONSENSUS; FAILURE DETECTOR; REPLICATION; SECURITY AB We present hBFT, a hybrid, Byzantine fault-tolerant, replicated state machine protocol with optimal resilience. Under normal circumstances, hBFT uses speculation, i.e., replicas directly adopt the order from the primary and send replies to the clients. As in prior work such as Zyzzyva, when replicas are out of order, clients can detect the inconsistency and help replicas converge on the total ordering. However, we take a different approach than previous work that has four distinct benefits: it requires many fewer cryptographic operations, it moves critical jobs to the clients with no additional costs, faulty clients can be detected and identified, and performance in the presence of client participation will not degrade as long as the primary is correct. The correctness is guaranteed by a three-phase checkpoint subprotocol similar to PBFT, which is tailored to our needs. The protocol is triggered by the primary when a certain number of requests are executed or by clients when they detect an inconsistency. C1 [Duan, Sisi; Peisert, Sean; Levitt, Karl N.] Univ Calif Davis, Dept Comp Sci, Davis, CA 95616 USA. [Peisert, Sean] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. RP Duan, S (reprint author), Univ Calif Davis, Dept Comp Sci, Davis, CA 95616 USA. EM sduan@cs.ucdavis.edu; peisert@cs.ucdavis.edu; levitt@cs.ucdavis.edu FU National Science Foundation [CCF-1018871] FX The authors would like to thank Matt Bishop, Jeff Rowe, Haibin Zhang, Hein Meling, Tiancheng Chang, and Leander Jehi for their helpful comments and contributions to the paper. This research was based on work supported by the National Science Foundation under Grant Number CCF-1018871. Any opinions, findings, and conclusions or recommendations expressed in this material are those of the authors and do not necessarily reflect those of the National Science Foundation. NR 33 TC 2 Z9 2 U1 0 U2 2 PU IEEE COMPUTER SOC PI LOS ALAMITOS PA 10662 LOS VAQUEROS CIRCLE, PO BOX 3014, LOS ALAMITOS, CA 90720-1314 USA SN 1545-5971 EI 1941-0018 J9 IEEE T DEPEND SECURE JI IEEE Trans. Dependable Secur. Comput. PD JAN-FEB PY 2015 VL 12 IS 1 BP 58 EP 70 DI 10.1109/TDSC.2014.2312331 PG 13 WC Computer Science, Hardware & Architecture; Computer Science, Information Systems; Computer Science, Software Engineering SC Computer Science GA CE7XC UT WOS:000352054200005 ER PT J AU Lund, CH Bromley, JR Stenbaek, A Rasmussen, RE Scheller, HV Sakuragi, Y AF Lund, Christian H. Bromley, Jennifer R. Stenbaek, Anne Rasmussen, Randi E. Scheller, Henrik V. Sakuragi, Yumiko TI A reversible Renilla luciferase protein complementation assay for rapid identification of protein-protein interactions reveals the existence of an interaction network involved in xyloglucan biosynthesis in the plant Golgi apparatus SO JOURNAL OF EXPERIMENTAL BOTANY LA English DT Article DE Arabidopsis thaliana; glycosyltransferase; Golgi apparatus; Nicotiana benthamiana; plant cell wall; polysaccharides; protein-protein interaction; Renilla luciferase; type II membrane protein; xyloglucan ID CELL-WALL BIOSYNTHESIS; GREEN FLUORESCENT PROTEIN; RESONANCE ENERGY-TRANSFER; GLUCAN SYNTHASE CSLC4; INTERACTIONS IN-VIVO; MEMBRANE-PROTEIN; GLUCURONOXYLAN BIOSYNTHESIS; UDP-ARABINOFURANOSE; FUNCTIONAL GENOMICS; ENZYME COMPLEXES AB A growing body of evidence suggests that protein-protein interactions (PPIs) occur amongst glycosyltransferases (GTs) required for plant glycan biosynthesis (e.g. cell wall polysaccharides and N-glycans) in the Golgi apparatus, and may control the functions of these enzymes. However, identification of PPIs in the endomembrane system in a relatively fast and simple fashion is technically challenging, hampering the progress in understanding the functional coordination of the enzymes in Golgi glycan biosynthesis. To solve the challenges, we adapted and streamlined a reversible Renilla luciferase protein complementation assay (Rluc-PCA), originally reported for use in human cells, for transient expression in Nicotiana benthamiana. We tested Rluc-PCA and successfully identified luminescence complementation amongst Golgi-localizing GTs known to form a heterodimer (GAUT1 and GAUT7) and those which homooligomerize (ARAD1). In contrast, no interaction was shown between negative controls (e.g. GAUT7, ARAD1, IRX9). Rluc-PCA was used to investigate PPIs amongst Golgi-localizing GTs involved in biosynthesis of hemicelluloses. Although no PPI was identified among six GTs involved in xylan biosynthesis, Rluc-PCA confirmed three previously proposed interactions and identified seven novel PPIs amongst GTs involved in xyloglucan biosynthesis. Notably, three of the novel PPIs were confirmed by a yeast-based split-ubiquitin assay. Finally, Gateway-enabled expression vectors were generated, allowing rapid construction of fusion proteins to the Rluc reporters and epitope tags. Our results show that Rluc-PCA coupled with transient expression in N. benthamiana is a fast and versatile method suitable for analysis of PPIs between Golgi resident proteins in an easy and mid-throughput fashion in planta. C1 [Lund, Christian H.; Bromley, Jennifer R.; Stenbaek, Anne; Rasmussen, Randi E.; Sakuragi, Yumiko] Univ Copenhagen, Dept Plant Biol & Biotechnol, DK-1871 Frederiksberg, Denmark. [Bromley, Jennifer R.; Scheller, Henrik V.] Joint BioEnergy Inst, Feedstocks Div, Emeryville, CA 94608 USA. [Bromley, Jennifer R.; Scheller, Henrik V.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 USA. [Scheller, Henrik V.] Univ Calif Berkeley, Dept Plant & Microbial Biol, Berkeley, CA 94720 USA. RP Sakuragi, Y (reprint author), Univ Copenhagen, Dept Plant Biol & Biotechnol, DK-1871 Frederiksberg, Denmark. EM ysa@plen.ku.dk RI Bromley, Jennifer/C-6632-2015; Scheller, Henrik/A-8106-2008; OI Scheller, Henrik/0000-0002-6702-3560; Bromley, Jennifer/0000-0002-2333-1238; Sakuragi, Yumiko/0000-0002-9405-5197 FU Danish Advanced Technology Foundation [001-2011-4]; Danish Council for Strategic Research [12-131834]; Nordic Research Energy (AquaFEED) [24]; European Union [ENERGY-2010-1, 256808]; People Programme Marie Curie Actions (PHOTO. COMM) [317184]; U.S. Department of Energy Office of Science; U.S. Department of Energy Office of Biological and Environmental Research [DE-AC02-05CH11231] FX This work was supported by the Danish Advanced Technology Foundation (Biomass for the 21st century, grant number 001-2011-4); The Danish Council for Strategic Research (Plant Power, grant number 12-131834); Nordic Research Energy (AquaFEED, grant number 24); European Union's Seventh Framework Programme FP7 (ENERGY-2010-1 DirectFuel, grant number 256808); The People Programme Marie Curie Actions (PHOTO. COMM, grant number 317184), and The U.S. Department of Energy Office of Science and Office of Biological and Environmental Research (contract no. DE-AC02-05CH11231 between Lawrence Berkeley National Laboratory and the U.S. Department of Energy). NR 71 TC 7 Z9 7 U1 4 U2 16 PU OXFORD UNIV PRESS PI OXFORD PA GREAT CLARENDON ST, OXFORD OX2 6DP, ENGLAND SN 0022-0957 EI 1460-2431 J9 J EXP BOT JI J. Exp. Bot. PD JAN PY 2015 VL 66 IS 1 BP 85 EP 97 DI 10.1093/jxb/eru401 PG 13 WC Plant Sciences SC Plant Sciences GA CE2QR UT WOS:000351660900008 PM 25326916 ER PT J AU Huang, JH Shkrob, IA Wang, PQ Cheng, L Pan, BF He, MN Liao, C Zhang, ZC Curtiss, LA Zhang, L AF Huang, Jinhua Shkrob, Ilya A. Wang, Peiqi Cheng, Lei Pan, Baofei He, Meinan Liao, Chen Zhang, Zhengcheng Curtiss, Larry A. Zhang, Lu TI 1,4-Bis(trimethylsilyl)-2,5-dimethoxybenzene: a novel redox shuttle additive for overcharge protection in lithium-ion batteries that doubles as a mechanistic chemical probe SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID ELECTROLYTE INTERFACE SEI; OVERDISCHARGE PROTECTION; RADICAL CATIONS; PERFORMANCE; DERIVATIVES; REDUCTION; CARBONATE; MATRICES; BENZENE; CELLS AB A novel redox shuttle additive, 1,4-bis(trimethylsilyl)-2,5-dimethoxybenzene (BTMSDB), is shown to deliver superb overcharge protection of LiFePO4 electrode in Li-ion batteries. Using this molecule as a chemical probe, we trace the cause of the eventual failure of this additive to the gradual loss of steric protection in the corresponding radical cation, providing the much needed mechanistic insight in the factors controlling the long-term efficiency of overcharge protection. C1 [Huang, Jinhua; Cheng, Lei; Pan, Baofei; Liao, Chen; Curtiss, Larry A.; Zhang, Lu] Argonne Natl Lab, Joint Ctr Energy Storage Res, Argonne, IL 60439 USA. [Huang, Jinhua; Shkrob, Ilya A.; Wang, Peiqi; Pan, Baofei; He, Meinan; Liao, Chen; Zhang, Zhengcheng; Zhang, Lu] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. [Cheng, Lei; Curtiss, Larry A.] Argonne Natl Lab, Div Mat Sci, Argonne, IL 60439 USA. RP Zhang, L (reprint author), Argonne Natl Lab, Joint Ctr Energy Storage Res, 9700 S Cass Ave, Argonne, IL 60439 USA. EM luzhang@anl.gov RI Pan, Baofei/H-2867-2015; OI Liao, Chen/0000-0001-5168-6493 FU U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences [DE-AC02-06CH11357]; Joint Center for Energy Storage Research (JCESR), an Energy Innovation Hub - U.S. Department of Energy, Office of Science, Basic Energy Sciences FX This work was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences under contract No. DE-AC02-06CH11357; it was also supported as part of the Joint Center for Energy Storage Research (JCESR), an Energy Innovation Hub funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences. NR 32 TC 12 Z9 13 U1 6 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 2015 VL 3 IS 14 BP 7332 EP 7337 DI 10.1039/c5ta00899a PG 6 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA CE5BR UT WOS:000351845400018 ER PT J AU Yang, ZZ Trahey, L Ren, Y Chan, MKY Lin, CK Okasinski, J Thackeray, MM AF Yang, Zhenzhen Trahey, Lynn Ren, Yang Chan, Maria K. Y. Lin, Chikai Okasinski, John Thackeray, Michael M. TI In situ high-energy synchrotron X-ray diffraction studies and first principles modeling of alpha-MnO2 electrodes in Li-O-2 and Li-ion coin cells SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID RECHARGEABLE LITHIUM BATTERIES; AIR BATTERIES; MANGANESE-DIOXIDE; OXYGEN BATTERIES; LI/AIR BATTERIES; CATALYST; CATHODE; ELECTROLYTES; PERSPECTIVE; STABILITY AB Despite their technological challenges, non-aqueous rechargeable lithium-oxygen cells offer extremely high theoretical energy densities and are therefore attracting much attention in a rapidly emerging area of electrochemical research. Early results have suggested that, among the transition metal oxides, alpha manganese dioxide (alpha-MnO2) appears to offer electrocatalytic properties that can enhance the electrochemical properties of Li-O-2 cells, particularly during the early cycles. In this study, we have investigated the hybrid Li-ion/Li-O-2 character of alpha-MnO2 electrodes in Li-O-2 coin cells by in situ high-energy synchrotron X-ray diffraction, and compared the results with conventional Li/alpha-MnO2 coin cells assembled under argon. Complementary first principles density functional theory calculations have been used to shed light on competing lithium insertion and lithium and oxygen insertion reactions within the alpha-MnO2 tunnel structure during discharge, relative to lithium peroxide or lithium oxide formation. C1 [Yang, Zhenzhen; Trahey, Lynn; Lin, Chikai; Thackeray, Michael M.] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. [Ren, Yang; Okasinski, John] Argonne Natl Lab, Adv Photon Source, Xray Sci Div, Argonne, IL 60439 USA. [Chan, Maria K. Y.] Argonne Natl Lab, Ctr Nanoscale Mat, Argonne, IL 60439 USA. RP Chan, MKY (reprint author), Argonne Natl Lab, Ctr Nanoscale Mat, 9700 S Cass Ave, Argonne, IL 60439 USA. EM mchan@anl.gov FU Center for Electrochemical Energy Science, an Energy Frontier Research Center - US Department of Energy, Office of Science, Basic Energy Sciences [DE-AC02-06CH11]; DOE [DE-AC02-06CH11357]; Center for Nanoscale Materials, a U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences User Facility [DE-AC02-06CH11357] FX This work was supported as a part of the Center for Electrochemical Energy Science, an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Basic Energy Sciences under award number DE-AC02-06CH11. Use of the Advanced Photon Source, a US DOE Office of Science User Facility operated by Argonne National Laboratory, was supported by DOE under Contract no. DE-AC02-06CH11357. 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. Naba K. Karan, Mahalingam Balasubramanian, Rick Spence and Charles Kurtz are thanked for their kind help with the in situ cell design and fabrication. NR 48 TC 8 Z9 8 U1 10 U2 60 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7488 EI 2050-7496 J9 J MATER CHEM A JI J. Mater. Chem. A PY 2015 VL 3 IS 14 BP 7389 EP 7398 DI 10.1039/c4ta06633b PG 10 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA CE5BR UT WOS:000351845400026 ER PT J AU King, G Ishida, K Page, K Fukuda, Y Albessard, AK Hattori, Y Hiramatsu, R Mitsuishi, I Okada, A Kato, M Fukushima, N AF King, Graham Ishida, Kunio Page, Katharine Fukuda, Yumi Albessard, Ariane Keiko Hattori, Yasushi Hiramatsu, Ryosuke Mitsuishi, Iwao Okada, Aoi Kato, Masahiro Fukushima, Noburu TI Cation and anion ordering in Sr2Si7Al3ON13 phosphors SO JOURNAL OF MATERIALS CHEMISTRY C LA English DT Article ID LIGHT-EMITTING-DIODES; WHITE LEDS; PHOTOLUMINESCENCE; GAS AB A series of photoluminescent Ce3+ doped samples with compositions close to Sr2Si7Al3ON13: Ce have been studied by neutron powder diffraction to determine the Si4+/Al3+ and N3-/O2- site ordering. Contrary to a commonly held assumption that the edge sharing tetrahedral sites in this structure are occupied exclusively by Al3+, we find a partial occupancy of Al3+ on these site but also an unexpected preference for Al3+ to occupy 2 other tetrahedral sites which are only corner sharing. From the crystal structures and local structures, as determined by pair distribution function (PDF) analysis, we also find evidence for alternating Si-Al site ordering within the edge sharing chains as well as dimerization of the Si4+ and Al3+ cations within these chains. The O2- are found to be partially ordered onto 2 of the anion sites, although small amounts of O2- are found on other sites as well. The cation and anion ordering found by neutron diffraction is supported by theoretical calculations. Understanding cation and anion ordering is essential for optimizing the photoluminescence properties of this promising class of phosphor materials. C1 [King, Graham; Page, Katharine] Los Alamos Natl Lab, Lujan Neutron Scattering Ctr, Los Alamos, NM 87545 USA. [Ishida, Kunio; Fukuda, Yumi; Albessard, Ariane Keiko; Hattori, Yasushi; Hiramatsu, Ryosuke; Mitsuishi, Iwao; Okada, Aoi; Kato, Masahiro; Fukushima, Noburu] Toshiba Co Ltd, Corp Res & Dev Ctr, Saiwai Ku, Kawasaki, Kanagawa 2128582, Japan. [Page, Katharine] Oak Ridge Natl Lab, Spallat Neutron Source, Oak Ridge, TN 37831 USA. RP King, G (reprint author), Los Alamos Natl Lab, Lujan Neutron Scattering Ctr, Los Alamos, NM 87545 USA. EM gking@lanl.gov; ishida@arl.rdc.toshiba.co.jp RI Page, Katharine/C-9726-2009; King, Graham/E-3632-2010 OI Page, Katharine/0000-0002-9071-3383; King, Graham/0000-0003-1886-7254 FU Los Alamos National Security, LLC under DOE [DE-AC52 06NA25396]; Toshiba Corporation FX This work benefited from the use of the HIPD and NPDF instruments at the Lujan Neutron Scattering Center at Los Alamos Neutron Science Center. Los Alamos National Laboratory is operated by Los Alamos National Security, LLC under DOE Contract No. DE-AC52 06NA25396. Funding for this project was provided by Toshiba Corporation. The authors are also grateful to M. Tohyama and M. Ezaki for valuable discussions. NR 20 TC 2 Z9 2 U1 1 U2 10 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7526 EI 2050-7534 J9 J MATER CHEM C JI J. Mater. Chem. C PY 2015 VL 3 IS 13 BP 3135 EP 3140 DI 10.1039/c5tc00060b PG 6 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA CE1VQ UT WOS:000351601200020 ER PT J AU Gu, PY Ma, Y He, JH Long, GK Wang, CY Chen, WQ Liu, Y Xu, QF Lu, JM Zhang, QC AF Gu, Pei-Yang Ma, Yong He, Jing-Hui Long, Guankui Wang, Chengyuan Chen, Wangqiao Liu, Yi Xu, Qing-Feng Lu, Jian-Mei Zhang, Qichun TI The substituent group effect on the morphology and memory performance of phenazine derivatives SO JOURNAL OF MATERIALS CHEMISTRY C LA English DT Article ID NONVOLATILE MEMORY; AQUEOUS-SOLUTION; THIN-FILM; DEVICES; MICROPARTICLES; NANOPARTICLES; HETEROACENE; COMPOUND; STORAGE AB In this paper, we focused on how the film morphology changes can affect the memory performance based on phenazine derivatives because the performance of many devices is strongly dependent on the morphology of organic molecules in the as-prepared films. To address this point, two phenazine derivatives, 7,8-bis(decyloxy)-3-(2-hydroxy-4,5-dinitrophenoxy) phenazin-2-ol (2OHPz) and 7,8-bis(decyloxy)3-( 2-(decyloxy)-4,5-dinitrophenoxy) phenazin-2-ol (1OHPz), have been successfully synthesized and characterized. These two compounds have the same electron-withdrawing groups (nitro and pyrazine) and molecular backbone, but different terminal substituted groups, which would be very helpful for us to understand how substituted groups affect the morphology and device performance. In fact, the sandwich-structured memory devices based on ITO/2OHPz/Al exhibited excellent ternary memory behavior with high ON2/ON1/OFF current ratios of 10(8.8)/10(3)/1 at switching threshold voltages of -1.80 V/-3.62 V while the memory devices based on ITO/1OHPz/Al displayed binary memory behavior with ON/OFF current ratios of 107.5/1 at a switching threshold voltage of -3.0 V. The different memory behaviors are attributed to the different molecular packing in the two phenazine derivatives, which is confirmed by AFM, XRD and UV-vis absorption. The AFM height image of the 2OHPz film thermally evaporated onto the ITO surface indicates the formation of self-organized fibril structures, which is in sharp contrast to that of the 1OHPz film. This variation suggests different degrees of aggregation in these films, which is also in accordance with the XRD and UV-vis absorption results. There is one diffraction peak at 2 theta 16.11 degrees for the film of 2OHPz, indicating the formation of a more ordered structure in the thin film. In contrast, there is no obvious diffraction peak in the film of 1OHPz. Moreover, the UV-vis absorption wavelength of the thin film of 2OHPz is blue-shifted by similar to 10 nm more than that of 1OHPz film compared to those in dichloromethane. C1 [Gu, Pei-Yang; Long, Guankui; Wang, Chengyuan; Chen, Wangqiao; Zhang, Qichun] Nanyang Technol Univ, Sch Mat Sci & Engn, Singapore 639798, Singapore. [Ma, Yong; He, Jing-Hui; Xu, Qing-Feng; Lu, Jian-Mei] Soochow Univ, Coll Chem Chem Engn & Mat Sci, Suzhou 215123, Peoples R China. [Liu, Yi] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mol Foundry & Adv Light Source, Berkeley, CA 94720 USA. [Zhang, Qichun] Nanyang Technol Univ, Div Chem & Biol Chem, Sch Phys & Math Sci, Singapore 637371, Singapore. RP Zhang, QC (reprint author), Nanyang Technol Univ, Sch Mat Sci & Engn, Singapore 639798, Singapore. EM xuqingfeng@suda.edu.cn; lujm@suda.edu.cn; qczhang@ntu.edu.sg RI zhang, qichun/A-2253-2011; Liu, yi/A-3384-2008; Foundry, Molecular/G-9968-2014; Wang, Chengyuan/G-3687-2016; OI Liu, yi/0000-0002-3954-6102; Long, Guankui/0000-0002-1826-3736 FU AcRF Tier 1 [RG 16/12]; MOE [ARC 20/12, ARC 2/13]; NRF FX P.-Y. Gu thanks Ms Tan Si Yu and Prof Yanli Zhao for helping us to test the HRMS. Q.Z. acknowledges financial support from AcRF Tier 1 (RG 16/12) and Tier 2 (ARC 20/12 and ARC 2/13) from MOE, and the CREATE program (Nanomaterials for Energy and Water Management) from NRF. NR 32 TC 8 Z9 8 U1 4 U2 21 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7526 EI 2050-7534 J9 J MATER CHEM C JI J. Mater. Chem. C PY 2015 VL 3 IS 13 BP 3167 EP 3172 DI 10.1039/c5tc00003c PG 6 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA CE1VQ UT WOS:000351601200024 ER PT S AU Loch, SD Ballance, CP Pindzola, MS Griffin, DC Colgan, JP Badnell, NR O'Mullane, MG AF Loch, S. D. Ballance, C. P. Pindzola, M. S. Griffin, D. C. Colgan, J. P. Badnell, N. R. O'Mullane, M. G. GP IOP TI Generalized Collisional Radiative Model for Light Elements: C: Data for the B Isonuclear Sequence SO LIGHT ELEMENT ATOM, MOLECULE AND RADICAL BEHAVIOUR IN THE DIVERTOR AND EDGE PLASMA REGIONS SE Journal of Physics Conference Series LA English DT Proceedings Paper CT Conference on Light Element Atom, Molecule and Radical Behaviour in the Divertor and Edge Plasma Regions CY NOV 18-MAR 22, 2009-2013 CL Vienna, AUSTRIA ID FINITE-DENSITY PLASMAS; DIELECTRONIC RECOMBINATION DATA; ELECTRON-IMPACT EXCITATION; ISOELECTRONIC SEQUENCE; R-MATRIX; HYDROGENIC IONS; IONIZATION; STATES; POPULATIONS; BORON AB A first stage collision database is assembled which contains electron-impact excitation, ionization, and recombination rate coefficients for B, B+, B2+, B3+, and B4+. The first stage database is constructed using the R-matrix with pseudostates, time-dependent close-coupling, and perturbative distorted-wave methods. A second stage collision database is then assembled which contains generalized collisional-radiative ionization, recombination, and power loss rate coefficients as a function of both temperature and density. The second stage database is constructed by solution of the collisional-radiative equations in the quasi-static equilibrium approximation using the first stage database. Both collision database stages reside in electronic form at the IAEA Labeled Atomic Data Interface (ALADDIN) database and the Atomic Data Analysis Structure (ADAS) open database. C1 [Loch, S. D.; Ballance, C. P.; Pindzola, M. S.] Auburn Univ, Dept Phys, Auburn, AL 36849 USA. [Griffin, D. C.] Dept Phys, Rollins Coll, Winter Pk, FL 32789 USA. [Colgan, J. P.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. [Badnell, N. R.; O'Mullane, M. G.] Univ Strathclyde, Dept Phys, Glasgow G4 0NG, Lanark, Scotland. RP Loch, SD (reprint author), Auburn Univ, Dept Phys, Auburn, AL 36849 USA. NR 26 TC 0 Z9 0 U1 1 U2 4 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2015 VL 576 AR 012004 DI 10.1088/1742-6596/576/1/012004 PG 19 WC Physics, Fluids & Plasmas; Physics, Multidisciplinary SC Physics GA BC3YP UT WOS:000352094600004 ER PT S AU Schultz, DR Stancil, PC Havener, CC AF Schultz, D. R. Stancil, P. C. Havener, C. C. GP IOP TI State-selective charge transfer cross sections for light ion impact of atomic hydrogen SO LIGHT ELEMENT ATOM, MOLECULE AND RADICAL BEHAVIOUR IN THE DIVERTOR AND EDGE PLASMA REGIONS SE Journal of Physics Conference Series LA English DT Proceedings Paper CT Conference on Light Element Atom, Molecule and Radical Behaviour in the Divertor and Edge Plasma Regions CY NOV 18-MAR 22, 2009-2013 CL Vienna, AUSTRIA ID SPECTROSCOPY; TEMPERATURE AB Owing to the utility of diagnosing plasma properties such as impurity concentration and spatial distribution, and plasma temperature and rotation, by detection of photon emission following capture of electrons from atomic hydrogen to excited states of multiply charged ions, new calculations of state-selective charge transfer involving light ions have been carried out using the atomic orbital close-coupling and the classical trajectory Monte Carlo methods. By comparing these with results of other approaches applicable in a lower impact energy regime, and by benchmarking them using key experimental data, knowledge of the cross sections can be made available across the range parameters needed by fusion plasma diagnostics. C1 [Schultz, D. R.] Univ N Texas, Dept Phys, Denton, TX 76203 USA. [Stancil, P. C.] Univ Georgia, Dept Phys & Astron, Athens, GA 30602 USA. [Havener, C. C.] Oak Ridge Natl Lab, Div Phys, Oak Ridge, TN 37831 USA. RP Schultz, DR (reprint author), Univ N Texas, Dept Phys, Denton, TX 76203 USA. NR 10 TC 0 Z9 0 U1 0 U2 0 PU IOP PUBLISHING LTD PI BRISTOL PA DIRAC HOUSE, TEMPLE BACK, BRISTOL BS1 6BE, ENGLAND SN 1742-6588 J9 J PHYS CONF SER PY 2015 VL 576 AR 012009 DI 10.1088/1742-6596/576/1/012009 PG 7 WC Physics, Fluids & Plasmas; Physics, Multidisciplinary SC Physics GA BC3YP UT WOS:000352094600009 ER PT J AU Terban, MW Johnson, M Di Michiel, M Billinge, SJL AF Terban, Maxwell W. Johnson, Matthew Di Michiel, Marco Billinge, Simon J. L. TI Detection and characterization of nanoparticles in suspension at low concentrations using the X-ray total scattering pair distribution function technique SO NANOSCALE LA English DT Article ID GOLD NANOPARTICLES; PLATINUM NANOPARTICLES; WATCHING NANOPARTICLES; PARTICLE GROWTH; PRUSSIAN BLUE; DIFFRACTION; EVOLUTION; KINETICS; PDF; NANOSTRUCTURE AB Difference atomic pair distribution function methods have been applied to detect and characterize nanoparticles suspended in a solvent at very dilute concentrations. We specifically consider nanoparticles of a pharmaceutical compound in aqueous solution using X-ray PDF methods, a challenging case due to the low atomic number of the nanoparticle species. The nanoparticles were unambiguously detected at the level of 0.25 wt%. Even at these low concentrations the signals were highly reproducible, allowing for reliable detection and quantitative analysis of the nanoparticle structure. C1 [Terban, Maxwell W.; Billinge, Simon J. L.] Columbia Univ, Dept Appl Phys & Appl Math, New York, NY 10027 USA. [Johnson, Matthew] GlaxoSmithKline Med Res Ctr, Stevenage SG1 2NY, Herts, England. [Di Michiel, Marco] ESRF, F-38043 Grenoble 9, France. [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 FU Laboratory Directed Research and Development (LDRD) program (Complex Modeling) at Brookhaven National Laboratory (BNL) - Office of Science, US Department of Energy (OS-DOE) [12-007, DE-SC00112704]; Columbia University Energy Frontier Research Center (EFRC) - U.S. Department of Energy, Basic Energy Sciences (DOE-BES) [DE-SC0001085] FX The authors thank M. Jamieson for help with the manuscript and acknowledge the ESRF for the award of in-house experimental time. Work in the S.J.L.B. group was supported by the Laboratory Directed Research and Development (LDRD) program 12-007 (Complex Modeling) at Brookhaven National Laboratory (BNL) which is supported by the Office of Science, US Department of Energy (OS-DOE), under Contract no. DE-SC00112704. M.T. was partially supported by the Columbia University Energy Frontier Research Center (EFRC) funded by the U.S. Department of Energy, Basic Energy Sciences (DOE-BES), under grant no. DE-SC0001085. NR 59 TC 8 Z9 8 U1 6 U2 30 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2040-3364 EI 2040-3372 J9 NANOSCALE JI Nanoscale PY 2015 VL 7 IS 12 BP 5480 EP 5487 DI 10.1039/c4nr06486k PG 8 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA CD8UR UT WOS:000351372400045 PM 25732228 ER PT J AU Pham, VH Gebre, T Dickerson, JH AF Viet Hung Pham Gebre, Tesfaye Dickerson, James H. TI Facile electrodeposition of reduced graphene oxide hydrogels for high-performance supercapacitors SO NANOSCALE LA English DT Article ID REDOX-ACTIVE ELECTROLYTE; ELECTROCHEMICAL CAPACITORS; ENERGY-STORAGE; DISPERSIONS AB We report both a facile, scalable method to prepare reduced graphene oxide hydrogels through the electrodeposition of graphene oxide and its use as an electrode for high-performance supercapacitors. Such systems exhibited specific capacitances of 147 and 223 F g(-1) at a current density of 10 A g(-1) when using H2SO4 and H2SO4 + hydroquinone redox electrolytes, respectively. C1 [Viet Hung Pham; Dickerson, James H.] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. [Gebre, Tesfaye] Florida A&M Univ, Dept Phys, Tallahassee, FL 32307 USA. RP Dickerson, JH (reprint author), Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. EM jdickerson@bnl.gov FU U.S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10886] FX This work was performed at the Center for Functional Nanomaterials, Brookhaven National Laboratory, which is supported by the U.S. Department of Energy, Office of Basic Energy Sciences, under Contract no. DE-AC02-98CH10886. NR 31 TC 10 Z9 10 U1 5 U2 58 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2040-3364 EI 2040-3372 J9 NANOSCALE JI Nanoscale PY 2015 VL 7 IS 14 BP 5947 EP 5950 DI 10.1039/c4nr07508k PG 4 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA CE6GL UT WOS:000351934700003 PM 25766250 ER PT J AU Pascal, TA Pemmaraju, CD Prendergast, D AF Pascal, Tod A. Pemmaraju, C. D. Prendergast, David TI X-ray spectroscopy as a probe for lithium polysulfide radicals SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID ABSORPTION-SPECTROSCOPY; SULFUR BATTERIES; ALKALI POLYSULFIDES; HIGH-CAPACITY; PSEUDOPOTENTIALS; DENSITY; CATHODE; ANION; HEXAMETHYLPHOSPHORAMIDE; DIFFRACTION AB The discharge mechanism in lithium sulfur batteries is still unknown and has been purported to involve significant concentrations of polysulfide radicals. Methods capable of quantifying these species in solution are therefore of paramount importance to revealing electrochemical pathways. Here we utilize DFT based X-ray Absorption Spectroscopy (XAS) simulations at the sulfur K-edge to obtain the spectra of polysulfide molecules in neutral, radical (-1) and dianionic (-2) charge states. Our calculations indicate that, contrary to recent propositions, the observed low energy, pre-edge feature in S K-edge XAS near 2470 eV is not exclusively due to radical species, but rather arises predominantly from core-excitations of terminal atoms, at the ends of linear polysulfides, to sigma* orbitals, consistent with our previous results for the dianionic species. We do however find a spectral feature unique to radicals, lying 0.5-1 eV below the established pre-edge, that arises from 1s -> pi* transitions of the terminal atoms. Existing measurements on polysulfides show no evidence for such transitions. We predict that detection of linear radicals in polysulfide mixtures using XAS is limited to high mole fractions (>20%), due to the relatively weak XAS intensity of this pi* feature. C1 [Pascal, Tod A.; Pemmaraju, C. D.; Prendergast, David] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA. RP Pascal, TA (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA. EM tod.a.cp@gmail.com; dgprendergast@lbl.gov RI Foundry, Molecular/G-9968-2014 FU Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the U.S. Department of Energy under the Batteries for Advanced Transportation Technologies (BATT) Program [DE-AC02-05CH11231]; Laboratory Directed Research and Development grant at Lawrence Berkeley National Laboratory; Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231]; Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231] FX During the review stage of this manuscript, we were alerted to an experimental study of dissolved lithium polysulfides in a working Li-S cell57 where the trisulfur radical was identified based on a low energy feature on the XAS near 2468.5 eV, exactly as predicted in this work. We thank reviewer #2 for bringing this to our attention. This work was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the U.S. Department of Energy under Contract DE-AC02-05CH11231 under the Batteries for Advanced Transportation Technologies (BATT) Program and a Laboratory Directed Research and Development grant at Lawrence Berkeley National Laboratory. Theory and simulations by TAP and DP were performed as part of a user project at the Molecular Foundry, Lawrence Berkeley National Laboratory supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. The methodology for spin-dependent spectral simulations was developed and implemented by CDP at the Molecular Foundry. Spectral simulations 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 57 TC 10 Z9 10 U1 9 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 2015 VL 17 IS 12 BP 7743 EP 7753 DI 10.1039/c4cp05316h PG 11 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA CD9SB UT WOS:000351437500019 PM 25714776 ER PT J AU Sun, CN Zawodzinski, TA Tenhaeff, WE Ren, F Keum, JK Bi, S Li, DW Ahn, SK Hong, KL Rondinone, AJ Carrillo, JMY Do, C Sumptergh, BG Chen, JH AF Sun, Che-Nan Zawodzinski, Thomas A., Jr. Tenhaeff, Wyatt E. Ren, Fei Keum, Jong Kahk Bi, Sheng Li, Dawen Ahn, Suk-Kyun Hong, Kunlun Rondinone, Adam J. Carrillo, Jan-Michael Y. Do, Changwoo Sumptergh, Bobby G. Chen, Jihua TI Nanostructure enhanced ionic transport in fullerene reinforced solid polymer electrolytes SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID METHYL-ESTER PCBM; POLY(ETHYLENE OXIDE); SOLAR-CELLS; CONDUCTIVITY BEHAVIOR; MECHANICAL-PROPERTIES; LITHIUM BATTERIES; CRYSTAL-STRUCTURE; MOLECULAR-WEIGHT; MORPHOLOGY; CRYSTALLIZATION AB Solid polymer electrolytes, such as polyethylene oxide (PEO) based systems, have the potential to replace liquid electrolytes in secondary lithium batteries with flexible, safe, and mechanically robust designs. Previously reported PEO nanocomposite electrolytes routinely use metal oxide nanoparticles that are often 5-10 nm in diameter or larger. The mechanism of those oxide particle-based polymer nanocomposite electrolytes is under debate and the ion transport performance of these systems is still to be improved. Herein we report a 6-fold ion conductivity enhancement in PEO/lithium bis(trifluoromethanesulfonyl) imide (LiTFSI)-based solid electrolytes upon the addition of fullerene derivatives. The observed conductivity improvement correlates with nanometer-scale fullerene crystallite formation, reduced crystallinities of both the (PEO) 6: LiTFSI phase and pure PEO, as well as a significantly larger PEO free volume. This improved performance is further interpreted by enhanced decoupling between ion transport and polymer segmental motion, as well as optimized permittivity and conductivity in bulk and grain boundaries. This study suggests that nanoparticle induced morphological changes, in a system with fullerene nanoparticles and no Lewis acidic sites, play critical roles in their ion conductivity enhancement. The marriage of fullerene derivatives and solid polymer electrolytes opens up significant opportunities in designing next-generation solid polymer electrolytes with improved performance. C1 [Sun, Che-Nan; Zawodzinski, Thomas A., Jr.] Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37831 USA. [Zawodzinski, Thomas A., Jr.] Univ Tennessee, Dept Chem & Biomol Engn, Knoxville, TN 37996 USA. [Tenhaeff, Wyatt E.] Univ Rochester, Dept Chem Engn, Rochester, NY 14627 USA. [Ren, Fei] Temple Univ, Dept Mech Engn, Philadelphia, PA 19122 USA. [Keum, Jong Kahk; Do, Changwoo] Oak Ridge Natl Lab, Neutron Scattering Sci Div, Oak Ridge, TN 37831 USA. [Bi, Sheng; Li, Dawen] Univ Alabama, Ctr Mat Informat Technol, Dept Elect & Comp Engn, Tuscaloosa, AL 35487 USA. [Ahn, Suk-Kyun; Hong, Kunlun; Rondinone, Adam J.; Carrillo, Jan-Michael Y.; Sumptergh, Bobby G.; Chen, Jihua] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. [Carrillo, Jan-Michael Y.; Sumptergh, Bobby G.] Oak Ridge Natl Lab, Comp Sci & Math Div, Oak Ridge, TN 37831 USA. RP Chen, JH (reprint author), Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. EM chenj1@ornl.gov RI Chen, Jihua/F-1417-2011; Hong, Kunlun/E-9787-2015; Sumpter, Bobby/C-9459-2013; Rondinone, Adam/F-6489-2013; Carrillo, Jan-Michael/K-7170-2013; Keum, Jong/N-4412-2015; Do, Changwoo/A-9670-2011 OI Chen, Jihua/0000-0001-6879-5936; Hong, Kunlun/0000-0002-2852-5111; Sumpter, Bobby/0000-0001-6341-0355; Rondinone, Adam/0000-0003-0020-4612; Carrillo, Jan-Michael/0000-0001-8774-697X; Keum, Jong/0000-0002-5529-1373; Do, Changwoo/0000-0001-8358-8417 FU NSF [CCS-1151140] FX This research was conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility. D. Li acknowledges travel support from NSF under award #ECCS-1151140. NR 48 TC 1 Z9 1 U1 7 U2 55 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2015 VL 17 IS 12 BP 8266 EP 8275 DI 10.1039/c4cp05583g PG 10 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA CD9SB UT WOS:000351437500076 PM 25733054 ER PT J AU Gul, S Ng, JWD Alonso-Mori, R Kern, J Sokaras, D Anzenberg, E Lassalle-Kaiser, B Gorlin, Y Weng, TC Zwart, PH Zhang, JZ Bergmann, U Yachandra, VK Jaramillo, TF Yano, J AF Gul, Sheraz Ng, Jia Wei Desmond Alonso-Mori, Roberto Kern, Jan Sokaras, Dimosthenis Anzenberg, Eitan Lassalle-Kaiser, Benedikt Gorlin, Yelena Weng, Tsu-Chien Zwart, Petrus H. Zhang, Jin Z. Bergmann, Uwe Yachandra, Vittal K. Jaramillo, Thomas F. Yano, Junko TI Simultaneous detection of electronic structure changes from two elements of a bifunctional catalyst using wavelength-dispersive X-ray emission spectroscopy and in situ electrochemistry SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID OXYGEN REDUCTION; PHOTOSYSTEM-II; ROOM-TEMPERATURE; WATER OXIDATION; FUEL-CELLS; CARBON; DIFFRACTION; PERFORMANCE; BIRNESSITE; CRYSTAL AB Multielectron catalytic reactions, such as water oxidation, nitrogen reduction, or hydrogen production in enzymes and inorganic catalysts often involve multimetallic clusters. In these systems, the reaction takes place between metals or metals and ligands to facilitate charge transfer, bond formation/breaking, substrate binding, and release of products. In this study, we present a method to detect X-ray emission signals from multiple elements simultaneously, which allows for the study of charge transfer and the sequential chemistry occurring between elements. K beta X-ray emission spectroscopy (XES) probes charge and spin states of metals as well as their ligand environment. A wavelength-dispersive spectrometer based on the von Hamos geometry was used to disperse K beta signals of multiple elements onto a position detector, enabling an XES spectrum to be measured in a single-shot mode. This overcomes the scanning needs of the scanning spectrometers, providing data free from temporal and normalization errors and therefore ideal to follow sequential chemistry at multiple sites. We have applied this method to study MnOx-based bifunctional electrocatalysts for the oxygen evolution reaction (OER) and the oxygen reduction reaction (ORR). In particular, we investigated the effects of adding a secondary element, Ni, to form MnNiOx and its impact on the chemical states and catalytic activity, by tracking the redox characteristics of each element upon sweeping the electrode potential. The detection scheme we describe here is general and can be applied to time-resolved studies of materials consisting of multiple elements, to follow the dynamics of catalytic and electron transfer reactions. C1 [Gul, Sheraz; Kern, Jan; Lassalle-Kaiser, Benedikt; Yachandra, Vittal K.; Yano, Junko] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 USA. [Gul, Sheraz; Zhang, Jin Z.] Univ Calif Santa Cruz, Dept Chem, Santa Cruz, CA 95060 USA. [Ng, Jia Wei Desmond; Gorlin, Yelena; Jaramillo, Thomas F.] Stanford Univ, Dept Chem Engn, Stanford, CA 94305 USA. [Alonso-Mori, Roberto; Kern, Jan; Sokaras, Dimosthenis; Weng, Tsu-Chien; Bergmann, Uwe] SLAC Natl Accelerator Lab, Menlo Pk, CA 94025 USA. [Anzenberg, Eitan; Jaramillo, Thomas F.; Yano, Junko] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Joint Ctr Artificial Photosynth, Berkeley, CA 94720 USA. [Zwart, Petrus H.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. RP Jaramillo, TF (reprint author), Stanford Univ, Dept Chem Engn, Stanford, CA 94305 USA. EM jaramillo@stanford.edu; jyano@lbl.gov RI Jaramillo, Thomas/C-4174-2014; OI Jaramillo, Thomas/0000-0001-9900-0622; Ng, Jia Wei Desmond/0000-0003-3196-9730 FU Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub; Office of Science of the U.S. Department of Energy [DE-SC0004993] FX XES experiments were supported by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the U.S. Department of Energy under Award Number DE-SC0004993, and performed at the Advanced Light Source (BL 5.0.2), Berkeley. The Berkeley Center for Structural Biology (BL 5.0.2) is supported in part by the National Institutes of Health, National Institute of General Medical Sciences, and the Howard Hughes Medical Institute. The Advanced Light Source is supported by the Director, Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. under Contract DE-AC02-05CH11231. Catalyst development and electrochemical characterization were supported as part of the Center on Nanostructuring for Efficient Energy Conversion (CNEEC) at Stanford University, 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-SC0001060. The development of the spectrometer was supported by the Director, Office of Science, Office of Basic Energy Sciences (OBES), Division of Chemical Sciences, Geosciences, and Biosciences (CSGB) of the Department of Energy (DOE) under Contract DEAC02- 05CH11231 (J. Y and V. K. Y.), and by the National Institute Of General Medical Sciences of the National Institutes of Health under Award Number R01GM110501 (J. Y.). Portions of this research (XAS data collection) were carried out at the Stanford Synchrotron Radiation Light source at BL 7-3, a Directorate of SLAC National Accelerator Laboratory and an Office of Science User Facility operated for the U. S. Department of Energy Office of Science by Stanford University. The SSRL Structural Molecular Biology Program is supported by the DOE Office of Biological and Environmental Research, and by the National Institutes of Health, National Institute of General Medical Sciences (including P41GM103393) and the National Center for Research Resources (P41RR001209). J. Z. Z. is grateful to the BES Division of the US Department of Energy for financial support. The authors thank Mr Jesse D. Benck for technical assistance. NR 37 TC 5 Z9 5 U1 4 U2 57 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2015 VL 17 IS 14 BP 8901 EP 8912 DI 10.1039/c5cp01023c PG 12 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA CE6GB UT WOS:000351933600043 PM 25747045 ER PT S AU Abernathy, DL Niedziela, JL Stone, MB AF Abernathy, D. L. Niedziela, J. L. Stone, M. B. BE Frick, B Koza, MM Boehm, M Mutka, H TI Extracting source parameters from beam monitors on a chopper spectrometer SO QENS/WINS 2014 - 11TH INTERNATIONAL CONFERENCE ON QUASIELASTIC NEUTRON SCATTERING AND 6TH INTERNATIONAL WORKSHOP ON INELASTIC NEUTRON SPECTROMETERS SE EPJ Web of Conferences LA English DT Proceedings Paper CT 11th International Conference on Quasielastic Neutron Scattering / 6th International Workshop on Inelastic Neutron Spectrometers (QENS/WINS) CY MAY 11-16, 2014 CL Autrans, FRANCE SP Inst LaueLangevin, ESS, FRMII, HZB, ILL, ISIS, JCNS, LLB, PSI AB The intensity distributions of beam monitors in direct-geometry time-of-flight neutron spectrometers provide important information about the instrument resolution. For short-pulse spallation neutron sources in particular, the asymmetry of the source pulse may be extracted and compared to Monte Carlo source simulations. An explicit formula using a Gaussian-convolved Ikeda-Carpenter distribution is given and compared to data from the ARCS instrument at the Spallation Neutron Source. C1 [Abernathy, D. L.; Stone, M. B.] Oak Ridge Natl Lab, Quantum Condensed Matter Div, Oak Ridge, TN 37831 USA. [Niedziela, J. L.] Oak Ridge Natl Lab, Instrument & Source Div, Oak Ridge, TN 37831 USA. RP Abernathy, DL (reprint author), Oak Ridge Natl Lab, Quantum Condensed Matter Div, Oak Ridge, TN 37831 USA. EM abernathydl@ornl.gov RI Stone, Matthew/G-3275-2011; Abernathy, Douglas/A-3038-2012; BL18, ARCS/A-3000-2012 OI Stone, Matthew/0000-0001-7884-9715; Abernathy, Douglas/0000-0002-3533-003X; NR 5 TC 1 Z9 1 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 J9 EPJ WEB CONF PY 2015 VL 83 AR 03001 DI 10.1051/epjconf/20158303001 PG 4 WC Physics, Multidisciplinary SC Physics GA BC3PN UT WOS:000351844900022 ER PT S AU Ehlers, G Stewart, JR Deen, PP Andersen, KH AF Ehlers, G. Stewart, J. R. Deen, P. P. Andersen, K. H. BE Frick, B Koza, MM Boehm, M Mutka, H TI Neutron xyz - polarization analysis at a time-of-flight instrument SO QENS/WINS 2014 - 11TH INTERNATIONAL CONFERENCE ON QUASIELASTIC NEUTRON SCATTERING AND 6TH INTERNATIONAL WORKSHOP ON INELASTIC NEUTRON SPECTROMETERS SE EPJ Web of Conferences LA English DT Proceedings Paper CT 11th International Conference on Quasielastic Neutron Scattering / 6th International Workshop on Inelastic Neutron Spectrometers (QENS/WINS) CY MAY 11-16, 2014 CL Autrans, FRANCE SP Inst LaueLangevin, ESS, FRMII, HZB, ILL, ISIS, JCNS, LLB, PSI ID SPECTROMETER; SCATTERING; MULTIDETECTOR AB When implementing a dedicated polarization analysis setup at a neutron time-of-flight instrument with a large area detector, one faces enormous challenges. Nevertheless, significant progress has been made towards this goal over the last few years. This paper addresses systematic limitations of the traditional method that is used to make these measurements, and a possible strategy to overcome these limitations. This will be important, for diffraction as well as inelastic experiments, where the scattering occurs mostly out-of-plane. C1 [Ehlers, G.] Oak Ridge Natl Lab, Quantum Condensed Matter Div, Oak Ridge, TN 37831 USA. [Stewart, J. R.] Rutherford Appleton Lab, ISIS, Didcot OX11 0QX, Oxon, England. [Deen, P. P.; Andersen, K. H.] European Spallat Source ESS AB, S-22100 Lund, Sweden. RP Ehlers, G (reprint author), Oak Ridge Natl Lab, Quantum Condensed Matter Div, Oak Ridge, TN 37831 USA. EM ehlersg@ornl.gov RI Stewart, Ross/C-4194-2008; Ehlers, Georg/B-5412-2008 OI Stewart, Ross/0000-0003-0053-0178; Ehlers, Georg/0000-0003-3513-508X NR 30 TC 0 Z9 0 U1 1 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 J9 EPJ WEB CONF PY 2015 VL 83 AR UNSP 03004 DI 10.1051/epjconf/20158303004 PG 6 WC Physics, Multidisciplinary SC Physics GA BC3PN UT WOS:000351844900025 ER PT S AU Granroth, GE Hahn, SE AF Granroth, G. E. Hahn, S. E. BE Frick, B Koza, MM Boehm, M Mutka, H TI Monte Carlo simulation of the resolution volume for the SEQUOIA spectrometer SO QENS/WINS 2014 - 11TH INTERNATIONAL CONFERENCE ON QUASIELASTIC NEUTRON SCATTERING AND 6TH INTERNATIONAL WORKSHOP ON INELASTIC NEUTRON SPECTROMETERS SE EPJ Web of Conferences LA English DT Proceedings Paper CT 11th International Conference on Quasielastic Neutron Scattering / 6th International Workshop on Inelastic Neutron Spectrometers (QENS/WINS) CY MAY 11-16, 2014 CL Autrans, FRANCE SP Inst LaueLangevin, ESS, FRMII, HZB, ILL, ISIS, JCNS, LLB, PSI ID NEUTRON-SCATTERING EXPERIMENTS; CHOPPER SPECTROMETER; MCSTAS; COMPUTATION; RESTRAX AB Monte Carlo ray tracing simulations, of direct geometry spectrometers, have been particularly useful in instrument design and characterization. However, these tools can also be useful for experiment planning and analysis. To this end, the McStas Monte Carlo ray tracing model of SEQUOIA, the fine resolution fermi chopper spectrometer at the Spallation Neutron Source (SNS) of Oak Ridge National Laboratory (ORNL), has been modified to include the time of flight resolution sample and detector components. With these components, the resolution ellipsoid can be calculated for any detector pixel and energy bin of the instrument. The simulation is split in two pieces. First, the incident beamline up to the sample is simulated for 1 x 10(11) neutron packets (4 days on 30 cores). This provides a virtual source for the backend that includes the resolution sample and monitor components. Next, a series of detector and energy pixels are computed in parallel. It takes on the order of 30 s to calculate a single resolution ellipsoid on a single core. Python scripts have been written to transform the ellipsoid into the space of an oriented single crystal, and to characterize the ellipsoid in various ways. Though this tool is under development as a planning tool, we have successfully used it to provide the resolution function for convolution with theoretical models. Specifically, theoretical calculations of the spin waves in YFeO3 were compared to measurements taken on SEQUOIA. Though the overall features of the spectra can be explained while neglecting resolution effects, the variation in intensity of the modes is well described once the resolution is included. As this was a single sharp mode, the simulated half intensity value of the resolution ellipsoid was used to provide the resolution width. A description of the simulation, its use, and paths forward for this technique will be discussed. C1 [Granroth, G. E.] Oak Ridge Natl Lab, Neutron Data Anal & Visualizat Div, Oak Ridge, TN 37831 USA. [Hahn, S. E.] Oak Ridge Natl Lab, Quantum Condensed Matter Div, Oak Ridge, TN 37831 USA. RP Granroth, GE (reprint author), Oak Ridge Natl Lab, Neutron Data Anal & Visualizat Div, Oak Ridge, TN 37831 USA. EM granrothge@ornl.gov RI Granroth, Garrett/G-3576-2012 OI Granroth, Garrett/0000-0002-7583-8778 NR 31 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 J9 EPJ WEB CONF PY 2015 VL 83 AR 03006 DI 10.1051/epjconf/20158303006 PG 4 WC Physics, Multidisciplinary SC Physics GA BC3PN UT WOS:000351844900027 ER PT S AU Grimaldo, M Roosen-Runge, F Jalarvo, N Zamponi, M Zanini, F Hennig, M Zhang, F Schreiber, F Seydel, T AF Grimaldo, Marco Roosen-Runge, Felix Jalarvo, Niina Zamponi, Michaela Zanini, Fabio Hennig, Marcus Zhang, Fajun Schreiber, Frank Seydel, Tilo BE Frick, B Koza, MM Boehm, M Mutka, H TI High-resolution neutron spectroscopy on protein solution samples SO QENS/WINS 2014 - 11TH INTERNATIONAL CONFERENCE ON QUASIELASTIC NEUTRON SCATTERING AND 6TH INTERNATIONAL WORKSHOP ON INELASTIC NEUTRON SPECTROMETERS SE EPJ Web of Conferences LA English DT Proceedings Paper CT 11th International Conference on Quasielastic Neutron Scattering / 6th International Workshop on Inelastic Neutron Spectrometers (QENS/WINS) CY MAY 11-16, 2014 CL Autrans, FRANCE SP Inst LaueLangevin, ESS, FRMII, HZB, ILL, ISIS, JCNS, LLB, PSI ID DYNAMICS; SCATTERING; DIFFUSION; POWDER AB Proteins in solution move subject to a complex superposition of global translational and rotational diffusion as well as internal relaxations covering a wide range of time scales. With the advent of new high-flux neutron spectrometers in combination with enhanced analysis frameworks it has become possible to separate these different contributions. We discuss new approaches to the analysis by presenting example spectra and fits from data recorded on the backscattering spectrometers IN16, IN16B, and BASIS on the same protein solution sample. We illustrate the separation of the rotational and translational diffusion contribution, the accurate treatment of the solvent contribution, and the extraction of information on internal fluctuations. We also exemplify the progress made in passing from second- to third-generation backscattering spectrometers. C1 [Grimaldo, Marco; Roosen-Runge, Felix; Hennig, Marcus; Seydel, Tilo] Inst Max von Laue Paul Langevin ILL, F-38042 Grenoble, France. [Grimaldo, Marco; Zanini, Fabio; Hennig, Marcus; Zhang, Fajun; Schreiber, Frank] Univ Tubingen, Inst Angew Phys, D-72076 Tubingen, Germany. [Jalarvo, Niina; Zamponi, Michaela] Forschungszentrum Julich, Julich Ctr Neutron Sci, D-52425 Julich, Germany. [Jalarvo, Niina] Oak Ridge Natl Lab, Spallat Neutron Source, JCNS Outstn, Oak Ridge, TN 37831 USA. [Zanini, Fabio] Max Planck Inst Dev Biol, D-72076 Tubingen, Germany. RP Grimaldo, M (reprint author), Inst Max von Laue Paul Langevin ILL, CS20156, F-38042 Grenoble, France. EM seydel@ill.eu RI Roosen-Runge, Felix/A-9107-2013; Jalarvo, Niina/Q-1320-2015; Schreiber, Frank/J-3311-2014; OI Roosen-Runge, Felix/0000-0001-5106-4360; Jalarvo, Niina/0000-0003-0644-6866; Schreiber, Frank/0000-0003-3659-6718; Zanini, Fabio/0000-0001-7097-8539 NR 23 TC 1 Z9 1 U1 1 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 J9 EPJ WEB CONF PY 2015 VL 83 AR 02005 DI 10.1051/epjconf/20158302005 PG 6 WC Physics, Multidisciplinary SC Physics GA BC3PN UT WOS:000351844900007 ER PT S AU Jalarvo, N Tyagi, M Crawford, MK AF Jalarvo, Niina Tyagi, Madhusudan Crawford, Michael K. BE Frick, B Koza, MM Boehm, M Mutka, H TI Quasielastic neutron scattering study of POSS ligand dynamics SO QENS/WINS 2014 - 11TH INTERNATIONAL CONFERENCE ON QUASIELASTIC NEUTRON SCATTERING AND 6TH INTERNATIONAL WORKSHOP ON INELASTIC NEUTRON SPECTROMETERS SE EPJ Web of Conferences LA English DT Proceedings Paper CT 11th International Conference on Quasielastic Neutron Scattering / 6th International Workshop on Inelastic Neutron Spectrometers (QENS/WINS) CY MAY 11-16, 2014 CL Autrans, FRANCE SP Inst LaueLangevin, ESS, FRMII, HZB, ILL, ISIS, JCNS, LLB, PSI AB Polyoligosilsesquioxanes are molecules having cage-like structures composed of silicon and oxygen. These molecules can have a wide variety of functional ligands attached to them. Depending on the nature of the ligand, interesting properties and applications are found. In this work we present results from quasielastic neutron scattering measurements of four different POSS molecules that illustrate the presence of strong coupling between the ligand dynamics and the POSS crystal structures. C1 [Jalarvo, Niina] Forschungszentrum Julich, Julich Ctr Neutron Sci, D-52428 Julich, Germany. [Jalarvo, Niina] Oak Ridge Natl Lab, Spallat Neutron Source, Chem & Engn Mat Div, Oak Ridge, TN 37861 USA. [Tyagi, Madhusudan] NIST, Ctr Neutron Res, Gaithersburg, MD 20899 USA. [Tyagi, Madhusudan] Univ Maryland, Dept Mat Sci, College Pk, MD 20742 USA. [Crawford, Michael K.] DuPont Cent Res & Dev, Wilmington, DE 19880 USA. RP Jalarvo, N (reprint author), Forschungszentrum Julich, Julich Ctr Neutron Sci, D-52428 Julich, Germany. EM n.jalarvo@fz-juelich.de RI Jalarvo, Niina/Q-1320-2015 OI Jalarvo, Niina/0000-0003-0644-6866 NR 8 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 J9 EPJ WEB CONF PY 2015 VL 83 AR 02007 DI 10.1051/epjconf/20158302007 PG 4 WC Physics, Multidisciplinary SC Physics GA BC3PN UT WOS:000351844900009 ER PT S AU Stone, MB Niedziela, JL Overbay, MA Abernathy, DL AF Stone, M. B. Niedziela, J. L. Overbay, M. A. Abernathy, D. L. BE Frick, B Koza, MM Boehm, M Mutka, H TI The ARCS radial collimator SO QENS/WINS 2014 - 11TH INTERNATIONAL CONFERENCE ON QUASIELASTIC NEUTRON SCATTERING AND 6TH INTERNATIONAL WORKSHOP ON INELASTIC NEUTRON SPECTROMETERS SE EPJ Web of Conferences LA English DT Proceedings Paper CT 11th International Conference on Quasielastic Neutron Scattering / 6th International Workshop on Inelastic Neutron Spectrometers (QENS/WINS) CY MAY 11-16, 2014 CL Autrans, FRANCE SP Inst LaueLangevin, ESS, FRMII, HZB, ILL, ISIS, JCNS, LLB, PSI ID NEUTRON-SCATTERING; SPECTROMETER AB We have designed, installed, and commissioned a scattered beam radial collimator for use at the ARCS Wide Angular Range Chopper Spectrometer at the Spallation Neutron Source. The collimator has been designed to work effectively for thermal and epithermal neutrons and with a range of sample environments. Other design considerations include the accommodation of working within a high vacuum environment and having the ability to quickly install and remove the collimator from the scattered beam. We present here characterization of the collimator's performance and methodologies for its effective use. C1 [Stone, M. B.; Abernathy, D. L.] Oak Ridge Natl Lab, Quantum Condensed Matter Sci Div, Oak Ridge, TN 37831 USA. [Niedziela, J. L.; Overbay, M. A.] Oak Ridge Natl Lab, Instrument & Source Div, Oak Ridge, TN 37831 USA. RP Stone, MB (reprint author), Oak Ridge Natl Lab, Quantum Condensed Matter Sci Div, Oak Ridge, TN 37831 USA. EM stonemb@ornl.gov RI Stone, Matthew/G-3275-2011; Abernathy, Douglas/A-3038-2012; BL18, ARCS/A-3000-2012 OI Stone, Matthew/0000-0001-7884-9715; Abernathy, Douglas/0000-0002-3533-003X; NR 9 TC 1 Z9 1 U1 2 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 J9 EPJ WEB CONF PY 2015 VL 83 AR 03014 DI 10.1051/epjconf/20158303014 PG 4 WC Physics, Multidisciplinary SC Physics GA BC3PN UT WOS:000351844900035 ER PT S AU Winn, B Filges, U Garlea, VO Graves-Brook, M Hagen, M Jiang, CY Kenzelmann, M Passell, L Shapiro, SM Tong, X Zaliznyak, I AF Winn, Barry Filges, Uwe Garlea, V. Ovidiu Graves-Brook, Melissa Hagen, Mark Jiang, Chenyang Kenzelmann, Michel Passell, Larry Shapiro, Stephen M. Tong, Xin Zaliznyak, Igor BE Frick, B Koza, MM Boehm, M Mutka, H TI Recent progress on HYSPEC, and its polarization analysis capabilities SO QENS/WINS 2014 - 11TH INTERNATIONAL CONFERENCE ON QUASIELASTIC NEUTRON SCATTERING AND 6TH INTERNATIONAL WORKSHOP ON INELASTIC NEUTRON SPECTROMETERS SE EPJ Web of Conferences LA English DT Proceedings Paper CT 11th International Conference on Quasielastic Neutron Scattering / 6th International Workshop on Inelastic Neutron Spectrometers (QENS/WINS) CY MAY 11-16, 2014 CL Autrans, FRANCE SP Inst LaueLangevin, ESS, FRMII, HZB, ILL, ISIS, JCNS, LLB, PSI ID SPALLATION NEUTRON SOURCE; HYBRID SPECTROMETER AB HYSPEC is a high-intensity, direct-geometry time-of-flight spectrometer at the Spallation Neutron Source, optimized for measurement of excitations in small single-crystal specimens with optional polarization analysis capabilities. The incident neutron beam is monochromated using a Fermi chopper with short, straight blades, and is then vertically focused by Bragg scattering onto the sample position by either a highly oriented pyrolitic graphite (unpolarized) or a Heusler (polarized) crystal array. Neutrons are detected by a bank of He-3 tubes that can be positioned over a wide range of scattering angles about the sample axis. HYSPEC entered the user program in February 2013 for unpolarized experiments, and is already experiencing a vibrant research program. Polarization analysis will be accomplished by using the Heusler crystal array to polarize the incident beam, and either a He-3 spin filter or a supermirror wide-angle polarization analyser to analyse the scattered beam. The He-3 spin filter employs the spin-exchange optical pumping technique. A 60 degrees wide angle He-3 cell that matches the detector coverage will be used for polarization analysis. The polarized gas in the post-sample wide angle cell is designed to be periodically and automatically refreshed with an adjustable pressure of polarized gas, optically pumped in a separate cell and then transferred to the wide angle cell. The supermirror analyser has 960 supermirror polarizers distributed over 60 degrees, and has been characterized at the Swiss Spallation Neutron Source. The current status of the instrument and the development of its polarization analysis capabilities are presented. C1 [Winn, Barry; Garlea, V. Ovidiu] Oak Ridge Natl Lab, Quantum Condensed Matter Div, Oak Ridge, TN 37831 USA. [Filges, Uwe; Kenzelmann, Michel] Paul Scherrer Inst, Lab Dev & Methods, Villigen, Switzerland. [Graves-Brook, Melissa; Jiang, Chenyang; Tong, Xin] Oak Ridge Natl Lab, Instrument & Source Div, Oak Ridge, TN USA. [Hagen, Mark] Oak Ridge Natl Lab, Neutron Data Anal & Visualizat, Oak Ridge, TN USA. [Hagen, Mark] European Spallat Source, Data Management & Software, Copenhagen, Denmark. [Passell, Larry; Shapiro, Stephen M.; Zaliznyak, Igor] Brookhaven Natl Lab, Condensed Matter Phys & Mat Sci Dept, Upton, NY 11973 USA. RP Winn, B (reprint author), Oak Ridge Natl Lab, Quantum Condensed Matter Div, Oak Ridge, TN 37831 USA. EM winnbl@ornl.gov RI Kenzelmann, Michel/A-8438-2008; Garlea, Vasile/A-4994-2016; Winn, Barry/A-5065-2016; tong, Xin/C-4853-2012; OI Kenzelmann, Michel/0000-0001-7913-4826; Garlea, Vasile/0000-0002-5322-7271; Winn, Barry/0000-0001-6383-4318; tong, Xin/0000-0001-6105-5345; Jiang, Chenyang/0000-0002-6321-3164 NR 10 TC 10 Z9 10 U1 2 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 J9 EPJ WEB CONF PY 2015 VL 83 AR 03017 DI 10.1051/epjconf/20158303017 PG 6 WC Physics, Multidisciplinary SC Physics GA BC3PN UT WOS:000351844900038 ER PT J AU Zou, JD Yan, M Yao, JL AF Zou, Junding Yan, Mi Yao, Jinlei TI The structural and magnetic properties of the compound Tm5Ge4 SO RSC ADVANCES LA English DT Article ID NEUTRON-DIFFRACTION; PHASE-RELATIONSHIPS; CRYSTAL-STRUCTURE; SYSTEM; GD-5(SIXGE1-X)(4); COEXISTENCE; TRANSITION; PRESSURE; SILICON; ALLOYS AB The compound Tm5Ge4 is the last one in the family of R5Ge4 (R = rare earth elements with magnetic moments) compounds (exclusive of Pm and Eu) whose magnetic properties are still unknown. We prepared high quality Tm5Ge4, and report the detailed crystal structure and magnetic properties. Tm5Ge4 crystallizes in the Sm5Ge4-type ortho-rhombic structure at room temperature, and orders antiferromagnetically at T-N' = 13 and T-N = 21 K. The paramagnetic Curie temperature of Tm5Ge4 is positive (theta(p) = 16 K), and the effective magnetic moment (p(eff) = 7.4 mu(B)/Tm) is in good agreement with the theoretical value of 7.56 mu(B)/Tm3+. The ac susceptibility of Tm5Ge4 shows obvious frequency dependence behaviors suggesting the existence of a ferromagnetic cluster in the antiferromagnetic substance. According to the magnetic hysteresis loop, the intrinsic coercivity of Tm5Ge4 is 2616 Oe at 2 K. Tm5Ge4 exhibits an oscillating magnetocaloric effect owing to a metamagnetic-like transformation induced by a critical magnetic field below 21 K. C1 [Zou, Junding; Yan, Mi] Zhejiang Univ, Key Lab Novel Mat Informat Technol Zhejiang Prov, State Key Lab Silicon Mat, Sch Mat Sci & Engn, Hangzhou 310027, Zhejiang, Peoples R China. [Zou, Junding] Iowa State Univ, US Dept Energy, Ames Lab, Ames, IA 50011 USA. [Yao, Jinlei] Suzhou Univ Sci & Technol, Sch Math & Phys, Res Ctr Solid State Phys & Mat, Suzhou 215009, Jiangsu, Peoples R China. RP Zou, JD (reprint author), Zhejiang Univ, Key Lab Novel Mat Informat Technol Zhejiang Prov, State Key Lab Silicon Mat, Sch Mat Sci & Engn, Hangzhou 310027, Zhejiang, Peoples R China. EM zoujd@zju.edu.cn; mse_yanmi@zju.edu.cn RI Yao, Jinlei/D-4977-2012 FU National Natural Science Foundation of China [51471150, 51301116]; Program for Innovative Research Team in University of Ministry of Education of China [IRT13R54]; U.S. Department of Energy, Office of Basic Energy Science, Division of Materials Sciences and Engineering; U.S. Department of Energy [DE-AC02-07CH11358] FX This work was supported by the National Natural Science Foundation of China (Grant no. 51471150, 51301116) and Program for Innovative Research Team in University of Ministry of Education of China (IRT13R54). Work at the Ames Laboratory was supported by the U.S. Department of Energy, Office of Basic Energy Science, Division of Materials Sciences and Engineering. The research was performed at the Ames Laboratory operated for the U.S. Department of Energy by Iowa State University under Contract no. DE-AC02-07CH11358. NR 44 TC 1 Z9 1 U1 3 U2 22 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2046-2069 J9 RSC ADV JI RSC Adv. PY 2015 VL 5 IS 34 BP 26850 EP 26855 DI 10.1039/c5ra02620b PG 6 WC Chemistry, Multidisciplinary SC Chemistry GA CE1FF UT WOS:000351556800051 ER PT J AU Mincher, BJ Schmitt, NC Schuetz, BK Shehee, TC Hobbs, DT AF Mincher, Bruce J. Schmitt, Nicholas C. Schuetz, Brian K. Shehee, Thomas C. Hobbs, David T. TI Recent advances in f-element separations based on a new method for the production of pentavalent americium in acidic solution SO RSC ADVANCES LA English DT Article ID ACTINIDE SEPARATIONS; SOLVENT-EXTRACTION; ION-EXCHANGE; LANTHANIDES; STRONTIUM; OXIDATION; MECHANISM; PHOSPHATE; KINETICS; CURIUM AB The peroxydisulfate anion has long been used for the preparation of hexavalent americium (Am-VI) from the normally stable Am-III valence state in mildly acidic solutions. However, there has been no satisfactory means to directly prepare the pentavalent state (Am-V) in that medium. Some early literature reports indicated that the peroxydisulfate oxidation was incomplete, and silver ion catalysis in conjunction with peroxydisulfate became accepted as the means to ensure quantitative generation of Am-VI. Incomplete oxidation would be expected to leave residual Am-III, or to produce Am-V in treated solutions. However, until recently, the use of peroxydisulfate as an Am-V reagent has not been reported. Here, parameters influencing the oxidation were investigated, including peroxydisulfate and acid concentration, temperature, duration of oxidative treatment, and the presence of higher concentrations of other redox active metals such as plutonium. Using optimized conditions determined here, quantitative Am-V was prepared in an acidic solution and the UV/Vis extinction coefficients of the Am-V 513 nm peak were measured over a range of nitric acid concentrations. The utility of Am-V for separations from the lanthanides and curium by solvent extraction, organic column chromatography and inorganic ion exchangers was also investigated. C1 [Mincher, Bruce J.; Schmitt, Nicholas C.; Schuetz, Brian K.] Idaho Natl Lab, Idaho Falls, ID 83415 USA. [Shehee, Thomas C.; Hobbs, David T.] Savannah River Natl Lab, Aiken, SC 29808 USA. RP Mincher, BJ (reprint author), Idaho Natl Lab, Idaho Falls, ID 83415 USA. EM bruce.mincher@inl.gov RI Mincher, Bruce/C-7758-2017 FU US DOE Office of Nuclear Energy Fuel Cycle R&D Sigma Team for Minor Actinide Separations Program under Idaho Operations [DE-AC07-05ID14517]; Savannah River Operations [DE-AC09-08SR22470] FX The INL and SRNL work was performed under the US DOE Office of Nuclear Energy Fuel Cycle R&D Sigma Team for Minor Actinide Separations Program under Idaho Operations Contract DE-AC07-05ID14517 and Savannah River Operations Contract DE-AC09-08SR22470. NR 29 TC 5 Z9 5 U1 1 U2 31 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2046-2069 J9 RSC ADV JI RSC Adv. PY 2015 VL 5 IS 34 BP 27205 EP 27210 DI 10.1039/c5ra03196f PG 6 WC Chemistry, Multidisciplinary SC Chemistry GA CE1FF UT WOS:000351556800099 ER PT J AU Xue, YP Jin, MJ Orjuela, A Slininger, PJ Dien, BS Dale, BE Balan, V AF Xue, Ya-Ping Jin, Mingjie Orjuela, Andrea Slininger, Patricia J. Dien, Bruce S. Dale, Bruce E. Balan, Venkatesh TI Microbial lipid production from AFEX (TM) pretreated corn stover SO RSC ADVANCES LA English DT Article ID CELLULOSIC ETHANOL-PRODUCTION; AMMONIA FIBER EXPANSION; CELL OIL PRODUCTION; LIGNOCELLULOSIC BIOMASS; OLEAGINOUS MICROORGANISMS; BIODIESEL; FERMENTATION; BIOCHEMISTRY; CHALLENGES AB Lipids having high carbon to heteroatom ratios can be upgraded to bio-diesel and jet fuels which are more advanced drop-in fuels compared to ethanol. The present study investigated microbial lipid production from Ammonia Fiber Expansion (AFEX) pretreated and hydrolyzed corn stover (CS) using an oleaginous yeast strain Lipomyces tetrasporus NRRL Y-11562. Process conditions were optimized for carbon to nitrogen ratio of fermentation medium, fermentation temperature and pH, and solid loading of AFEX-CS. The inhibitory effect of AFEX degradation products on lipid fermentation was also investigated. Both separate hydrolysis and fermentation (SHF) and Rapid Bioconversion with Integrated recycle Technology (RaBIT) processes were used for lipid production. From 1 kg AFEX-CS, 36.7 g lipids were produced via SHF at a titer of 8.4 g L-1 with a yield of 0.08 g g(-1) consumed sugar. A yeast meal stream (97.9 g) was also generated. L. tetrasporus NRRL Y-11562 grew better in AFEX-CS hydrolysate, but produced fewer lipids compared to synthetic medium. Minimal washing of AFEX-CS improved the lipid yield and titer to 0.10 g g(-1) consumed sugar and 10.7 g L-1, respectively. RaBIT on washed AFEX-CS generated a similar amount of lipids compared to SHF with 35% lower enzyme loading. Economic analysis does not favor lignocellulosic lipid production with current lipid yields. C1 [Xue, Ya-Ping; Jin, Mingjie; Orjuela, Andrea; Dale, Bruce E.; Balan, Venkatesh] Michigan State Univ, Dept Chem Engn & Mat Sci, Biomass Convers Res Lab BCRL, Lansing, MI 48910 USA. [Xue, Ya-Ping] Zhejiang Univ Technol, Inst Bioengn, Hangzhou 310014, Zhejiang, Peoples R China. [Jin, Mingjie; Orjuela, Andrea; Dale, Bruce E.; Balan, Venkatesh] Michigan State Univ, DOE Great Lakes Bioenergy Res Ctr GLBRC, E Lansing, MI 48824 USA. [Slininger, Patricia J.; Dien, Bruce S.] ARS, Natl Ctr Agr Utilizat Res, USDA, Peoria, IL 61604 USA. RP Jin, MJ (reprint author), Michigan State Univ, Dept Chem Engn & Mat Sci, Biomass Convers Res Lab BCRL, MBI Bldg,3815 Technol Blvd, Lansing, MI 48910 USA. EM jinmingj@egr.msu.edu FU China Scholarship Council FX This work is supported by the China Scholarship Council. We would like to thank Novozymes for supplying us commercial enzymes for this work, Charles Donald Jr for preparing AFEX-pretreated corn stover and Christa Gunawan for analyzing HPLC samples. We would also like to thank the members of the Biomass Conversion Research Laboratory (BCRL) at Michigan State University for their valuable suggestions. We also thank Dr Cletus P. Kurtzman for supplying the culture for this research. NR 30 TC 4 Z9 4 U1 6 U2 26 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2046-2069 J9 RSC ADV JI RSC Adv. PY 2015 VL 5 IS 36 BP 28725 EP 28734 DI 10.1039/c5ra01134e PG 10 WC Chemistry, Multidisciplinary SC Chemistry GA CE5JY UT WOS:000351870500087 ER PT J AU Bazilevskaya, E Rother, G Mildner, DFR Pavich, M Cole, D Bhatt, MP Jin, LX Steefel, CI Brantley, SL AF Bazilevskaya, Ekaterina Rother, Gernot Mildner, David F. R. Pavich, Milan Cole, David Bhatt, Maya P. Jin, Lixin Steefel, Carl I. Brantley, Susan L. TI How Oxidation and Dissolution in Diabase and Granite Control Porosity during Weathering SO SOIL SCIENCE SOCIETY OF AMERICA JOURNAL LA English DT Article ID SMALL-ANGLE SCATTERING; NEUTRON-SCATTERING; VIRGINIA PIEDMONT; FRACTAL GEOMETRY; SAPONITE SERIES; PUERTO-RICO; ROCKS; REPLACEMENT; EVOLUTION; REGOLITH AB Weathering extends to shallower depths on diabase than granite ridgetops despite similar climate and geomorphological regimes of denudation in the Virginia (United States) Piedmont. Deeper weathering has been attributed to advective transport of solutes in granitic rock compared to diffusive transport in diabase. We use neutron scattering (NS) techniques to quantify the total and connected submillimeter porosity (nominal diameters between 1 nm and 10 mm) and specific surface area (SSA) during weathering. The internal surface of each unweathered rock is characterized as both a mass fractal and a surface fractal. The mass fractal describes the distribution of pores (similar to 300 nm to similar to 5 mu m) along grain boundaries and triple junctions. The surface fractal is interpreted as the distribution of smaller features (1-300 nm), that is, the bumps (or irregularities) at the grain-pore interface. The earliest porosity development in the granite is driven by microfracturing of biotite, which leads to the introduction of fluids that initiate dissolution of other silicates. Once plagioclase weathering begins, porosity increases significantly and the mass + surface fractal typical for unweathered granite transforms to a surface fractal as infiltration of fluids continues. In contrast, the mass + surface fractal does not transform to a surface fractal during weathering of the diabase, perhaps consistent with the interpretation that solute transport is dominated by diffusion in that rock. The difference in regolith thickness between granite and diabase is likely due to the different mechanisms of solute transport across the primary silicate reaction front. C1 [Bazilevskaya, Ekaterina; Brantley, Susan L.] Penn State Univ, Earth & Environm Syst Inst, University Pk, PA 16802 USA. [Rother, Gernot] Oak Ridge Natl Lab, Div Chem Sci, Geochem & Interfacial Sci Grp, Oak Ridge, TN 37831 USA. [Mildner, David F. R.] NIST, NIST Ctr Neutron Res, Gaithersburg, MD 20899 USA. [Pavich, Milan] US Geol Survey, Eastern Geol & Paleoclimate Sci Ctr, Reston, VA 20192 USA. [Cole, David] Ohio State Univ, Sch Earth Sci, Columbus, OH 43219 USA. [Bhatt, Maya P.] Tribhuvan Univ, Cent Dep Environm Sci, Kathmandu, Nepal. [Jin, Lixin] Univ Texas El Paso, Dept Geol Sci, El Paso, TX 79968 USA. [Steefel, Carl I.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. RP Bazilevskaya, E (reprint author), Penn State Univ, Earth & Environm Syst Inst, University Pk, PA 16802 USA. EM eab204@psu.edu RI Steefel, Carl/B-7758-2010; Rother, Gernot/B-7281-2008 OI Rother, Gernot/0000-0003-4921-6294 FU DOE [DE-FG02-05ER15675]; Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy; Department of Energy Office of Basic Energy Sciences, Energy Frontier Research Center, "Nanoscale Control of Geologic CO2"; Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231]; National Science Foundation [DMR-0944772] FX This project was funded by DOE Grant DE-FG02-05ER15675. The research of GR was sponsored by the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy. DRC was supported by the Department of Energy Office of Basic Energy Sciences as part of an Energy Frontier Research Center, "Nanoscale Control of Geologic CO2" led by Lawrence Berkeley National Laboratory. The Advanced Light Source is supported by the Director, Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract DE-AC02-05CH11231. We specifically acknowledge Duluth Parkinson for the help with tomography imaging at beamline 8.3.2 at the Advanced Light Source at Lawrence Berkeley National Laboratory. The small-angle neutron scattering at the National Institute of Standards and Technology, U.S. Department of Commerce, was supported in part by the National Science Foundation under Agreement DMR-0944772. Transmission electron microscopy and SEM work was done at Materials Research Institute, Penn State. The identification of commercial instruments in this paper does not imply recommendation or endorsement by the National Institute of Standards and Technology, nor does it imply that the equipment used are necessarily the best available for the purpose. NR 64 TC 9 Z9 9 U1 3 U2 18 PU SOIL SCI SOC AMER PI MADISON PA 677 SOUTH SEGOE ROAD, MADISON, WI 53711 USA SN 0361-5995 EI 1435-0661 J9 SOIL SCI SOC AM J JI Soil Sci. Soc. Am. J. PD JAN-FEB PY 2015 VL 79 IS 1 BP 55 EP 73 DI 10.2136/sssaj2014.04.0135 PG 19 WC Soil Science SC Agriculture GA CE2JB UT WOS:000351640800007 ER PT S AU Bourgin, D Courtin, S Haas, F Goasduff, A Stefanini, AM Montagnoli, G Montanari, D Corradi, L Huiming, J Scarlassara, F Fioretto, E Simenel, C Rowley, N Jiang, CL Szilner, S Mijatovic, T AF Bourgin, D. Courtin, S. Haas, F. Goasduff, A. Stefanini, A. M. Montagnoli, G. Montanari, D. Corradi, L. Huiming, J. Scarlassara, F. Fioretto, E. Simenel, C. Rowley, N. Jiang, C. L. Szilner, S. Mijatovic, T. BE Simenel, C Gomes, PRS Hinde, DJ Madhavan, N Navin, A Rehm, KE TI Exploring the influence of transfer channels on fusion reactions: the case of Ca-40+Ni-58,Ni-64 SO VI INTERNATIONAL CONFERENCE FUSION14 SE EPJ Web of Conferences LA English DT Proceedings Paper CT 6th International Conference on FUSION CY FEB 24-28, 2014 CL New Delhi, INDIA ID NI-58 AB Fusion cross sections have been measured in the Ca-40 + Ni-58 and Ca-40 + Ni-64 systems at beam energies ranging from Elab = 104.75 MeV to 153.5 MeV using the Laboratori Nazionali di Legnaro electrostatic deflector. Distributions of barriers have been extracted from the experimental data. Preliminary coupled channel calculations were performed and hints of effects of neutron transfers on the fusion below the barrier in the Ca-40 + Ni-64 are discussed. C1 [Bourgin, D.; Courtin, S.; Haas, F.; Goasduff, A.; Montanari, D.] CNRS, IN2P3, Inst Pluridisciplinaire Hubert Curien, UMR7178, F-67037 Strasbourg, France. [Stefanini, A. M.; Corradi, L.; Huiming, J.; Fioretto, E.] Ist Nazl Fis Nucl, Lab Nazl Legnaro, I-35020 Legnaro, Padova, Italy. [Montagnoli, G.; Scarlassara, F.] Univ Padua, Dipartimento Fis, I-35131 Padua, Italy. [Montagnoli, G.; Scarlassara, F.] Ist Nazl Fis Nucl, I-35131 Padua, Italy. [Simenel, C.] Australian Natl Univ, RSPE, Dept Nucl Phys, Canberra, ACT 2601, Australia. [Rowley, N.] Inst Phys Nucl, F-91406 Orsay, France. [Jiang, C. L.] Argonne Natl Lab, Argonne, IL 60439 USA. [Szilner, S.; Mijatovic, T.] Rudjer Boskovic Inst, HR-10002 Zagreb, Croatia. RP Courtin, S (reprint author), CNRS, IN2P3, Inst Pluridisciplinaire Hubert Curien, UMR7178, 23 Rue Loess, F-67037 Strasbourg, France. EM sandrine.courtin@iphc.cnrs.fr RI Simenel, Cedric/H-3705-2014 OI Simenel, Cedric/0000-0002-2356-7769 NR 13 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 J9 EPJ WEB CONF PY 2015 VL 86 AR 00005 DI 10.1051/epjconf/20158600005 PG 3 WC Physics, Multidisciplinary; Physics, Nuclear SC Physics GA BC3PF UT WOS:000351833700005 ER PT S AU Stefanini, AM Montagnoli, G Esbensen, H Corradi, L Courtin, S Fioretto, E Goasduff, A Grebosz, J Haas, F Mazzocco, M Michelagnoli, C Mijatovic, T Montanari, D Pasqualato, G Parascandolo, C Scarlassara, F Strano, E Szilner, S Toniolo, N Torresi, D AF Stefanini, A. M. Montagnoli, G. Esbensen, H. Corradi, L. Courtin, S. Fioretto, E. Goasduff, A. Grebosz, J. Haas, F. Mazzocco, M. Michelagnoli, C. Mijatovic, T. Montanari, D. Pasqualato, G. Parascandolo, C. Scarlassara, F. Strano, E. Szilner, S. Toniolo, N. Torresi, D. BE Simenel, C Gomes, PRS Hinde, DJ Madhavan, N Navin, A Rehm, KE TI Transfer couplings and hindrance far below the barrier for Ca-40+Zr-96 SO VI INTERNATIONAL CONFERENCE FUSION14 SE EPJ Web of Conferences LA English DT Proceedings Paper CT 6th International Conference on FUSION CY FEB 24-28, 2014 CL New Delhi, INDIA ID FUSION AB The sub-barrier fusion excitation function of Ca-40 + Zr-96 has been measured down to cross sections similar or equal to 2.4 mu b, i.e. two orders of magnitude smaller than obtained in the previous experiment, where the sub-barrier fusion of this system was found to be greatly enhanced with respect to Ca-40 + Zr-90, and the need of coupling to transfer channels was suggested. The purpose of this work was to investigate the behavior of Ca-40 + Zr-96 fusion far below the barrier. The smooth trend of the excitation function has been found to continue, and the logarithmic slope increases very slowly. No indication of hindrance shows up, and a comparison with Ca-48 + Zr-96 is very useful in this respect. A new CC analysis of the complete excitation function has been performed, including explicitly one- and two-nucleon Q > 0 transfer channels. Such transfer couplings bring significant cross section enhancements, even at the level of a few mu b. Locating the hindrance threshold, if any, in Ca-40 + Zr-96 would require challenging measurements of cross sections in the sub-mu b range. C1 [Stefanini, A. M.; Corradi, L.; Fioretto, E.; Toniolo, N.] Ist Nazl Fis Nucl, Lab Nazl Legnaro, I-35020 Padua, Italy. [Montagnoli, G.; Mazzocco, M.; Michelagnoli, C.; Montanari, D.; Pasqualato, G.; Parascandolo, C.; Scarlassara, F.; Strano, E.; Torresi, D.] Univ Padua, Dipartimento Fis & Astron, I-35131 Padua, Italy. [Montagnoli, G.; Mazzocco, M.; Michelagnoli, C.; Montanari, D.; Pasqualato, G.; Parascandolo, C.; Scarlassara, F.; Strano, E.; Torresi, D.] Ist Nazl Fis Nucl, Sez Padova, I-35131 Padua, Italy. [Esbensen, H.] Argonne Natl Lab, Div Phys, Argonne, IL 60439 USA. [Courtin, S.; Haas, F.] Univ Strasbourg, CNRS, IN2P3, IPHC, F-67037 Strasbourg 2, France. [Goasduff, A.] CNRS, IN2P3, CSNSM, F-91405 Orsay, France. [Goasduff, A.] Univ Paris 11, F-91405 Orsay, France. [Grebosz, J.] Polish Acad Sci, Inst Nucl Phys, PL-31342 Krakow, Poland. [Mijatovic, T.] Rudjer Boskovic Inst, HR-10002 Zagreb, Croatia. RP Stefanini, AM (reprint author), Ist Nazl Fis Nucl, Lab Nazl Legnaro, I-35020 Padua, Italy. EM alberto.stefanini@lnl.infn.it OI Scarlassara, Fernando/0000-0002-4663-8216 NR 19 TC 0 Z9 0 U1 0 U2 6 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 J9 EPJ WEB CONF PY 2015 VL 86 AR 00056 DI 10.1051/epjconf/20158600056 PG 4 WC Physics, Multidisciplinary; Physics, Nuclear SC Physics GA BC3PF UT WOS:000351833700056 ER PT J AU An, K Somorjai, GA AF An, Kwangjin Somorjai, Gabor A. TI Nanocatalysis I: Synthesis of Metal and Bimetallic Nanoparticles and Porous Oxides and Their Catalytic Reaction Studies SO CATALYSIS LETTERS LA English DT Article DE Nanocatalysis; Mesoporous; Bimetallic; Core/shell; Strong-metal support interaction; Selectivity ID GENERATION VIBRATIONAL SPECTROSCOPY; SINGLE-CRYSTAL SURFACES; SHAPE CONTROL; CORE-SHELL; PLATINUM NANOPARTICLES; PYRROLE HYDROGENATION; BENZENE HYDROGENATION; SUPPORT INTERACTIONS; PARTICLE-SIZE; N-HEXANE AB In recent heterogeneous catalysis, much effort has been made in understanding how the size, shape, and composition of nanoparticles and oxide-metal interfaces affect catalytic performance at the molecular level. Recent advances in colloidal synthetic techniques enable preparing diverse metallic or bimetallic nanoparticles with well-defined size, shape, and composition and porous oxides as a high surface support. As nanoparticles become smaller, new chemical, physical, and catalytic properties emerge. Geometrically, as the smaller the nanoparticle the greater the relative number of edge and corner sites per unit surface of the nanoparticle. When the nanoparticles are smaller than a critical size (2.7 nm), finite-size effects such as a change of adsorption strength or oxidation state are revealed by changes in their electronic structures. By alloying two metals, the formation of heteroatom bonds and geometric effects such as strain due to the change of metal-metal bond lengths cause new electronic structures to appear in bimetallic nanoparticles. Ceaseless catalytic reaction studies have been discovered that the highest reaction yields, product selectivity, and process stability were achieved by determining the critical size, shape, and composition of nanoparticles and by choosing the appropriate oxide support. Depending on the pore size, various kinds of micro-, meso-, and macro-porous materials are fabricated by the aid of structure-directing agents or hard-templates. Recent achievements for the preparation of versatile core/shell nanostructures composing mesoporous oxides, zeolites, and metal organic frameworks provide new insights toward nanocatalysis with novel ideas. C1 [An, Kwangjin; Somorjai, Gabor A.] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [An, Kwangjin; Somorjai, Gabor A.] Lawrence Berkeley Natl Lab, Chem Sci Div, Berkeley, CA 94720 USA. [An, Kwangjin; Somorjai, Gabor A.] Lawrence Berkeley Natl Lab, Mat Sci Div, Berkeley, CA 94720 USA. RP Somorjai, GA (reprint author), Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. EM somorjai@berkeley.edu RI Foundry, Molecular/G-9968-2014 FU Director, Office of Basic Energy Sciences, Materials Science and Engineering Division of the U.S. Department of Energy [DE-AC02-05CH11231]; Chevron Corporation. FX This work was supported by the Director, Office of Basic Energy Sciences, Materials Science and Engineering Division of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. The user project at the Advanced Light Source and the Molecular Foundry of the Lawrence Berkeley National Laboratory, a DOE Office of Science User Facility. The nanoparticle synthesis was funded by Chevron Corporation. We thank Walter Ralston for correcting the proof.3 NR 72 TC 20 Z9 20 U1 16 U2 96 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1011-372X EI 1572-879X J9 CATAL LETT JI Catal. Lett. PD JAN PY 2015 VL 145 IS 1 BP 233 EP 248 DI 10.1007/s10562-014-1399-x PG 16 WC Chemistry, Physical SC Chemistry GA AY7BT UT WOS:000347717000028 ER PT J AU Alayoglu, S Somorjai, GA AF Alayoglu, Selim Somorjai, Gabor A. TI Nanocatalysis II: In Situ Surface Probes of Nano-Catalysts and Correlative Structure-Reactivity Studies SO CATALYSIS LETTERS LA English DT Article DE In situ NEXAFS; APXPS; In situ SFG; Environmental transmission electron microscopy; Metal-support interaction; Spillover ID SUM-FREQUENCY GENERATION; ENHANCED RAMAN-SPECTROSCOPY; FISCHER-TROPSCH SYNTHESIS; RAY-ABSORPTION-SPECTROSCOPY; TEMPERATURE CO OXIDATION; HIGH GAS-PRESSURES; ENERGY ION-SCATTERING; FT-IR SPECTROSCOPY; REAL-TIME PROBE; 3D ATOM-PROBE AB Model nano-catalysts with monodisperse particle sizes and architectures are essential for a fundamental understanding of surface property dynamics during catalytic reactions. Surface tools and techniques, when conducted under catalytically relevant temperature and pressure conditions, render possible measurements of dynamic surface properties such as oxidation state, composition, coordination, and bonding. Near edge X-ray absorption fine structure (NEXAFS) spectroscopy with purposely built in situ reaction cells and ambient pressure X-ray photoelectron spectroscopy (APXPS) provide (near) surface sensitive and chemical specific information on the oxidation states of metal and oxide (co-)catalysts as well as adsorbent functional elements such C, O and N under reactive gas atmospheres and even liquid environments. Likewise, sum frequency generation (SFG) vibrational spectroscopy with in situ reaction cells helps uncover the bonding geometry and configuration of the topmost surface again under conditions pertinent to catalysis. Furthermore, the local dynamics in the nanoscale and on the single particle level are revealed by environmental transmission electron microscopy (ETEM) and the spectro-microscopy techniques equipped within. A correlative approach, where an array of these in situ tools and techniques were conducted in parallel with catalytic measurements, was employed to gain molecular insight into some of the modern scientific challenges in heterogeneous catalysis. Several case examples of this correlative approach are presented here. The CO oxidation reaction over hybrid nano-catalysts of Pt nanoparticles (NPs) with various mesoporous metal oxides such as Co3O4, MnO2 and CeO2 was explored in relation to bifunctional catalysis and interfacial charge transfer chemistry by using in situ NEXAFS spectroscopy. Likewise, bimetallic CoPt and PtSn nanoparticle catalysts supported on silica were investigated by using a combination of in situ NEXAFS spectroscopy and APXPS. Next, CO2 hydrogenation was carried out over bimetallic CoPt/SiO2 and Co/TiO2 hybrid nano-catalysts. In this case, in situ NEXAFS spectroscopy, APXPS, and ETEM indicated severe, yet reversible, surface restructuring that involved hydrogen atom spillover. Finally, similar to 2 nm Pt NPs were investigated using in situ SFG to study hydrogenation and hydrogenative isomerization reactions. Specifically, SFG indicated that the hydrogenation of furfural and crotonaldehyde proceed by interfacial hydrogen atom spillover from TiO2, while the hydrogenative isomerization of methylcyclopentane (MCP) proceeds by spillover and surface diffusion of cyclohexene over mesoporous zeolites. These studies unequivocally indicated the presence of a particular reaction channel that involved one way flow of charged (i.e. electrons or protons) or neutral species (i.e. reactants) at a broadly defined interface between metals and oxides. In addition to these case studies, experimental approaches employing capillary flow micro-reactors are discussed in relation toward the goal of short time resolutions that could help isolate such charged or neutral intermediates in the future. C1 [Alayoglu, Selim; Somorjai, Gabor A.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Chem Sci Div, Berkeley, CA USA. [Alayoglu, Selim; Somorjai, Gabor A.] Univ Calif Berkeley, Dept Chem, Berkeley, CA USA. RP Somorjai, GA (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Chem Sci Div, Berkeley, CA USA. EM salayoglu@lbl.gov; somorjai@berkeley.edu RI Foundry, Molecular/G-9968-2014 FU Materials Science Division (MSD) at the Lawrence Berkeley National Laboratory; Director, Office of Energy Research, Office of Basic Energy Sciences of the U.S. Department of Energy [DE-AC02-05CH1123] FX Instrument part of this work was funded by the Materials Science Division (MSD) at the Lawrence Berkeley National Laboratory. The research in the MSD; and the user projects in the Advanced Light Source, Molecular Foundry and National Center for Electron Microscopy were supported by the Director, Office of Energy Research, Office of Basic Energy Sciences of the U.S. Department of Energy under Contract DE-AC02-05CH1123. NR 120 TC 5 Z9 5 U1 24 U2 120 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1011-372X EI 1572-879X J9 CATAL LETT JI Catal. Lett. PD JAN PY 2015 VL 145 IS 1 BP 249 EP 271 DI 10.1007/s10562-014-1398-y PG 23 WC Chemistry, Physical SC Chemistry GA AY7BT UT WOS:000347717000029 ER PT J AU Mittal, S Vetter, JS AF Mittal, Sparsh Vetter, Jeffrey S. TI A Survey of Methods for Analyzing and Improving GPU Energy Efficiency SO ACM COMPUTING SURVEYS LA English DT Article DE Experimentation; Management; Measurement; Performance; Analysis; GPU (graphics-processing unit); energy saving; power management; energy efficiency; architecture techniques; power model; green computing ID REGISTER FILE; POWER; PERFORMANCE; PROCESSOR; SYSTEMS; COMPUTATION; TRADEOFFS; SELECTION; CACHE AB Recent years have witnessed phenomenal growth in the computational capabilities and applications of GPUs. However, this trend has also led to a dramatic increase in their power consumption. This article surveys research works on analyzing and improving energy efficiency of GPUs. It also provides a classification of these techniques on the basis of their main research idea. Further, it attempts to synthesize research works that compare the energy efficiency of GPUs with other computing systems (e.g., FPGAs and CPUs). The aim of this survey is to provide researchers with knowledge of the state of the art in GPU power management and motivate them to architect highly energy-efficient GPUs of tomorrow. C1 [Mittal, Sparsh] Iowa State Univ, Ames, IA USA. [Vetter, Jeffrey S.] Oak Ridge Natl Lab, Future Technol Grp, Oak Ridge, TN 37830 USA. [Vetter, Jeffrey S.] Georgia Tech, Atlanta, GA USA. RP Mittal, S (reprint author), Oak Ridge Natl Lab, Future Technol Grp, 1 Bethel Valley Rd,Bldg 5100,MS-6173, Oak Ridge, TN 37830 USA. EM mittals@ornl.gov; vetter@ornl.gov FU UT-Battelle, LLC [DE-AC05-00OR22725]; Office of Advanced Scientific Computing Research in the U.S. Department of Energy FX The work was performed when Sparsh Mittal was at Iowa State University. The article has been authored by Oak Ridge National Laboratory, which is managed by UT-Battelle, LLC under Contract #DE-AC05-00OR22725 to the U.S. government. Accordingly, the U.S. government retains a nonexclusive, royalty-free license to publish or reproduce the published form of this contribution, or allow others to do so, for U.S. government purposes. This research is sponsored by the Office of Advanced Scientific Computing Research in the U.S. Department of Energy. NR 145 TC 5 Z9 5 U1 0 U2 9 PU ASSOC COMPUTING MACHINERY PI NEW YORK PA 2 PENN PLAZA, STE 701, NEW YORK, NY 10121-0701 USA SN 0360-0300 EI 1557-7341 J9 ACM COMPUT SURV JI ACM Comput. Surv. PD JAN PY 2015 VL 47 IS 2 AR 19 DI 10.1145/2636342 PG 23 WC Computer Science, Theory & Methods SC Computer Science GA CD9SE UT WOS:000351437800005 ER PT J AU Singh, A Taylor, LE Vander Wall, TA Linger, J Himmel, ME Podkaminer, K Adney, WS Decker, SR AF Singh, Arjun Taylor, Larry E., II Vander Wall, Todd A. Linger, Jeffrey Himmel, Michael E. Podkaminer, Kara Adney, William S. Decker, Stephen R. TI Heterologous protein expression in Hypocrea jecorina: A historical perspective and new developments SO BIOTECHNOLOGY ADVANCES LA English DT Review DE Trichoderma reesei; Hypocrea jecorina; QM6a; Rut-C30; cbh1; Cel7A; Cellobiohydrolase; cbh1 deletion; Fungal transformation; Cellulase expression systems ID FUNGUS TRICHODERMA-REESEI; STEP GENE REPLACEMENT; BETA-GLUCOSIDASE GENE; CELLOBIOHYDROLASE-I; TRANSFORMATION SYSTEM; SACCHAROMYCES-CEREVISIAE; HORMOCONIS-RESINAE; FILAMENTOUS FUNGI; PICHIA-PASTORIS; GLUCOAMYLASE-P AB Hypocrea jecorina, the sexual teleomorph of Trichoderma reesei, has long been favored as an industrial cellulase producer, first utilizing its native cellulase system and later augmented by the introduction of heterologous enzymatic activities or improved variants of native enzymes. Expression of heterologous proteins in H. jecorina was once considered difficult when the target was an improved variant of a native cellulase. Developments over the past nearly 30 years have produced strains, vectors, and selection mechanisms that have continued to simplify and streamline heterologous protein expression in this fungus. More recent developments in fungal molecular biology have pointed the way toward a fundamental transformation in the ease and efficiency of heterologous protein expression in this important industrial host. Here, I) we provide a historical perspective on advances in H. jecorina molecular biology, 2) outline host strain engineering, transformation, selection, and expression strategies, 3) detail potential pitfalls when working with this organism, and 4) provide consolidated examples of successful cellulase expression outcomes from our laboratory. (C) 2014 Published by Elsevier Inc. C1 [Singh, Arjun; Linger, Jeffrey] Natl Renewable Energy Lab, Natl Bioenergy Ctr, Golden, CO 80401 USA. [Taylor, Larry E., II; Vander Wall, Todd A.; Himmel, Michael E.; Podkaminer, Kara; Adney, William S.; Decker, Stephen R.] Natl Renewable Energy Lab, Biosci Ctr, Golden, CO 80401 USA. RP Decker, SR (reprint author), NREL, 15013 Denver West Pkwy, Golden, CO 80401 USA. EM Steve.decker@nrel.gov FU U.S. Department of Energy [DE-AC36-08GO28308]; National Renewable Energy Laboratory; DOE Office of Energy Efficiency and Renewable Energy, Bioenergy Technologies Office FX This work was supported by the U.S. Department of Energy under Contract No. DE-AC36-08GO28308 with the National Renewable Energy Laboratory. Funding for the work was provided by the DOE Office of Energy Efficiency and Renewable Energy, Bioenergy Technologies Office. NR 107 TC 7 Z9 7 U1 6 U2 23 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0734-9750 EI 1873-1899 J9 BIOTECHNOL ADV JI Biotechnol. Adv. PD JAN-FEB PY 2015 VL 33 IS 1 BP 142 EP 154 DI 10.1016/j.biotechadv.2014.11.009 PG 13 WC Biotechnology & Applied Microbiology SC Biotechnology & Applied Microbiology GA CD8BY UT WOS:000351321400010 PM 25479282 ER PT S AU Solecki, W Rosenzweig, C Blake, R de Sherbinin, A Matte, T Moshary, F Rosenzweig, B Arend, M Gaffin, S Bou-Zeid, E Rule, K Sweeny, G Dessy, W AF Solecki, William Rosenzweig, Cynthia Blake, Reginald de Sherbinin, Alex Matte, Tom Moshary, Fred Rosenzweig, Bernice Arend, Mark Gaffin, Stuart Bou-Zeid, Elie Rule, Keith Sweeny, Geraldine Dessy, Wendy BE Rosenzweig, C Solecki, W TI New York City Panel on Climate Change 2015 Report Chapter 6: Indicators and Monitoring SO BUILDING THE KNOWLEDGE BASE FOR CLIMATE RESILIENCY: NEW YORK CITY PANEL ON CLIMATE CHANGE 2015 REPORT SE Annals of the New York Academy of Sciences LA English DT Article; Book Chapter ID MANAGEMENT; SHIFTS C1 [Solecki, William] CUNY, Inst Sustainable Cities, New York, NY 10021 USA. [Rosenzweig, Cynthia] Columbia Univ, Climate Impacts Grp, NASA Goddard Inst Space Studies, Ctr Climate Syst Res,Earth Inst, New York, NY USA. [Blake, Reginald] CUNY, Dept Phys, New York City Coll Technol, Brooklyn, NY 11210 USA. [Blake, Reginald] NASA, Goddard Inst Space Studies, Climate Impacts Grp, Washington, DC 20546 USA. [de Sherbinin, Alex] Columbia Univ, CIESIN, Palisades, NY USA. [Matte, Tom] New York City Dept Hlth & Mental Hyg, New York, NY USA. [Moshary, Fred; Arend, Mark] CUNY, City Coll New York, NOAA CREST, New York, NY 10021 USA. [Rosenzweig, Bernice] CUNY, CUNY Environm Crossrd, City Coll New York, New York, NY 10021 USA. [Gaffin, Stuart] Columbia Univ, Earth Inst, Ctr Climate Syst Res, New York, NY USA. [Bou-Zeid, Elie] Princeton Univ, Dept Civil & Environm Engn, Princeton, NJ 08544 USA. [Rule, Keith] Princeton Univ, Plasma Phys Lab, Princeton, NJ USA. [Sweeny, Geraldine; Dessy, Wendy] New York City Mayors Off Operat, New York, NY USA. RP Solecki, W (reprint author), CUNY Hunter Coll, Dept Geog, New York, NY 10021 USA. OI de Sherbinin, Alex/0000-0002-8875-4864 NR 49 TC 2 Z9 2 U1 0 U2 5 PU BLACKWELL SCIENCE PUBL PI OXFORD PA OSNEY MEAD, OXFORD OX2 0EL, ENGLAND SN 0077-8923 J9 ANN NY ACAD SCI JI Ann.NY Acad.Sci. PY 2015 VL 1336 BP 89 EP 106 DI 10.1111/nyas.12587 PG 18 WC Environmental Sciences SC Environmental Sciences & Ecology GA BC3EX UT WOS:000351586900010 PM 25688948 ER PT J AU Durham, JL Kirshenbaum, K Takeuchi, ES Marschilok, AC Takeuchi, KJ AF Durham, Jessica L. Kirshenbaum, Kevin Takeuchi, Esther S. Marschilok, Amy C. Takeuchi, Kenneth J. TI Synthetic control of composition and crystallite size of silver ferrite composites: profound electrochemistry impacts SO CHEMICAL COMMUNICATIONS LA English DT Article ID HYDROTHERMAL SYNTHESIS; DELAFOSSITE STRUCTURE; PRE-EDGE; K-EDGE; IRON; MAGNETITE; FE; COORDINATION; HOLLANDITE; CHEMISTRY AB A paradigm for concomitant control of crystallite size and composition of bimetallic composites via co-precipitation is introduced. Direct preparation of composites of silver ferrite and amorphous maghemite via nonstoichiometric synthesis was demonstrated. Notable impact on electrochemistry was observed, with similar to 200% increase in reversible capacity for the small crystallite material. C1 [Durham, Jessica L.; Takeuchi, Esther S.; Marschilok, Amy C.; Takeuchi, Kenneth J.] SUNY Stony Brook, Dept Chem, Stony Brook, NY 11794 USA. [Kirshenbaum, Kevin; Takeuchi, Esther S.] Brookhaven Natl Lab, Upton, NY 11973 USA. [Takeuchi, Esther S.; Marschilok, Amy C.; Takeuchi, Kenneth J.] SUNY Stony Brook, Dept Mat Sci & Engn, Stony Brook, NY 11794 USA. RP Takeuchi, KJ (reprint author), SUNY Stony Brook, Dept Chem, Stony Brook, NY 11794 USA. EM kenneth.takeuchi.1@stonybrook.edu FU Department of Energy (DOE), Office of Basic Energy Sciences (BES) [DE-SC0008512]; Gertrude and Maurice Goldhaber Distinguished Fellowship Program; DOE, Office of Science, BES [DE-AC02-98CH10886] FX The authors acknowledge the Department of Energy (DOE), Office of Basic Energy Sciences (BES), under Grant DE-SC0008512. K. Kirshenbaum acknowledges the Gertrude and Maurice Goldhaber Distinguished Fellowship Program. X-ray absorption spectra were collected on beam line X11A at Brookhaven National Laboratory's National Synchrotron Light Source (NSLS), supported by the DOE, Office of Science, BES, under Contract No. DE-AC02-98CH10886. The authors acknowledge K. Pandya for assistance with XAS. NR 33 TC 6 Z9 6 U1 0 U2 36 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1359-7345 EI 1364-548X J9 CHEM COMMUN JI Chem. Commun. PY 2015 VL 51 IS 24 BP 5120 EP 5123 DI 10.1039/c4cc10277k PG 4 WC Chemistry, Multidisciplinary SC Chemistry GA CD6TI UT WOS:000351221900042 PM 25714656 ER PT J AU Liu, GK AF Liu, Guokui TI Advances in the theoretical understanding of photon upconversion in rare-earth activated nanophosphors SO CHEMICAL SOCIETY REVIEWS LA English DT Review ID ORBIT-LATTICE RELAXATION; NEAR-INFRARED EMISSION; CRYSTAL-FIELD ANALYSIS; ENERGY-TRANSFER; CONFIGURATION-INTERACTION; LANTHANIDE IONS; SPECTROSCOPIC PROPERTIES; DIELECTRIC PARTICLES; EXCITED-STATES; ANTI-STOKES AB Photon upconversion in rare earth activated phosphors involves multiple mechanisms of electronic transitions. Stepwise optical excitation, energy transfer, and various nonlinear and collective light-matter interaction processes act together to convert low-energy photons into short-wavelength light emission. Upconversion luminescence from nanomaterials exhibits additional size and surface dependencies. A fundamental understanding of the overall performance of an upconversion system requires basic theories on the spectroscopic properties of solids containing rare earth ions. This review article surveys the recent progress in the theoretical interpretations of the spectroscopic characteristics and luminescence dynamics of photon upconversion in rare earth activated phosphors. The primary aspects of upconversion processes, including energy level splitting, transition probability, line broadening, nonradiative relaxation and energy transfer, are covered with an emphasis on interpreting experimental observations. Theoretical models and methods for analyzing nano-phenomena in upconversion are introduced with detailed discussions on recently reported experimental results. C1 Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. RP Liu, GK (reprint author), Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM gkliu@anl.gov FU US Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences [DE-AC02-06CH11357]; CAS/SAFEA International Partnership Program for Creative Research Teams FX This material is based upon work supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, under contract DE-AC02-06CH11357. The author acknowledges travel support from the CAS/SAFEA International Partnership Program for Creative Research Teams. NR 102 TC 46 Z9 46 U1 24 U2 120 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 0306-0012 EI 1460-4744 J9 CHEM SOC REV JI Chem. Soc. Rev. PY 2015 VL 44 IS 6 BP 1635 EP 1652 DI 10.1039/c4cs00187g PG 18 WC Chemistry, Multidisciplinary SC Chemistry GA CD7BI UT WOS:000351244800015 PM 25286989 ER PT J AU Chan, EM AF Chan, Emory M. TI Combinatorial approaches for developing upconverting nanomaterials: high-throughput screening, modeling, and applications SO CHEMICAL SOCIETY REVIEWS LA English DT Review ID UP-CONVERSION LUMINESCENCE; RARE-EARTH IONS; TRANSMISSION ELECTRON-MICROSCOPY; LANTHANIDE-DOPED NANOPARTICLES; CONVERTING PHOSPHOR REPORTERS; SIZE-EXCLUSION CHROMATOGRAPHY; CORE-SHELL NANOPARTICLES; PAR TRANSFERT DENERGIE; UN TUNGSTATE MIXTE; ENERGY-TRANSFER AB Colloidal nanoparticles doped with lanthanide ions can upconvert near-infrared light to visible frequencies, enabling the application of such materials to biological imaging and luminescent solar concentration. The optical properties of upconverting nanomaterials are determined by their combination of lanthanide dopants, by their morphology, by their host matrices, and by their surface ligands. Identifying ideal compositions and synthesis conditions for these materials can be tedious and time-consuming due to the large number of parameters to optimize. This review surveys the use of combinatorial strategies to rapidly screen and optimize diverse libraries of upconverting nanomaterials. I will review high-throughput techniques for synthesizing and characterizing large libraries of nanocrystals, and I will discuss theoretical methods for modeling the optical properties of lanthanide-doped materials. Case studies will illustrate the use of these approaches for optimizing the physical properties of upconverting nanoparticles, including cases in which unexpected phenomena were revealed. Finally, this review will identify promising opportunities in which combinatorial techniques could accelerate on-going research or facilitate the discovery of novel upconverting nanomaterials that overcome fundamental limitations of current material designs. C1 Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA. RP Chan, EM (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA. EM EMChan@lbl.gov RI Foundry, Molecular/G-9968-2014 FU Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy (DOE) [DE-AC02-05CH11231] FX Work at the Molecular Foundry, Lawrence Berkeley National Laboratory was supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy (DOE) under Contract No. DE-AC02-05CH11231. The author acknowledges D. Hsieh for valuable input on this manuscript; C. Dodson and R. Zia for assistance with calculations; and E. Levy, A. Gotlin, J. Lee, C. Guan, J. Goldberg, J. Urban, D. Milliron, B. Cohen, and J. Schuck for helpful discussions and contributions to this research. NR 234 TC 31 Z9 31 U1 22 U2 116 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 0306-0012 EI 1460-4744 J9 CHEM SOC REV JI Chem. Soc. Rev. PY 2015 VL 44 IS 6 BP 1653 EP 1679 DI 10.1039/c4cs00205a PG 27 WC Chemistry, Multidisciplinary SC Chemistry GA CD7BI UT WOS:000351244800016 PM 25287124 ER PT J AU Kumar, G Swaminathan, S AF Kumar, Gyanendra Swaminathan, Subramanyam TI Recent Developments with Metalloprotease Inhibitor Class of Drug Candidates for Botulinum Neurotoxins SO CURRENT TOPICS IN MEDICINAL CHEMISTRY LA English DT Review DE Bioterrorism; Clostridium botulinum; Drug discovery; Neurotoxin; Protease inhibitor ID LIGHT-CHAIN PROTEASE; CLOSTRIDIUM-BOTULINUM; SMALL-MOLECULE; SEROTYPE-A; SUBSTRATE RECOGNITION; PROTEOLYTIC ACTIVITY; POTENT INHIBITORS; SNAP-25 SUBSTRATE; INFANT BOTULISM; TOXIN AB Botulinum Neurotoxins are the most poisonous of all toxins with lethal dose in nanogram quantities. They are potential biological warfare and bioterrorism agents due to their high toxicity and ease of preparation. On the other hand BoNTs are also being increasingly used for therapeutic and cosmetic purposes, and with that the chances of accidental overdose are increasing. And despite the potential damage they could cause to human health, there are no post-intoxication drugs available so far. But progress is being made in this direction. The crystal structures in native form and bound with substrate peptides have been determined, and these are enabling structure-based drug discovery possible. High throughput assays have also been designed to speed up the screening progress. Substrate-based and small molecule inhibitors have been identified. But turning high affinity inhibitors into clinically viable drug candidates has remained a challenge. We discuss here the latest developments and the future challenges in drug discovery for Botulinum neurotoxins. C1 [Kumar, Gyanendra; Swaminathan, Subramanyam] Brookhaven Natl Lab, Biol Environm & Climate Sci Dept, Upton, NY 11973 USA. [Kumar, Gyanendra] St Jude Childrens Res Hosp, Dept Struct Biol, Memphis, TN USA. RP Swaminathan, S (reprint author), Brookhaven Natl Lab, Biol Environm & Climate Sci Dept, 50 Bell Ave,Bldg 463, Upton, NY 11973 USA. EM Gyanendra.Kumar@StJude.Org; swami@bnl.gov FU DTRA under DOE prime [BO742081, DEAC02-98CH10886]; Brookhaven National Laboratory FX Research was supported by an award from DTRA BO742081 under DOE prime contract No. DEAC02-98CH10886 (PI: SS) with Brookhaven National Laboratory. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. NR 76 TC 4 Z9 4 U1 2 U2 7 PU BENTHAM SCIENCE PUBL LTD PI SHARJAH PA EXECUTIVE STE Y-2, PO BOX 7917, SAIF ZONE, 1200 BR SHARJAH, U ARAB EMIRATES SN 1568-0266 EI 1873-4294 J9 CURR TOP MED CHEM JI Curr. Top. Med. Chem. PY 2015 VL 15 IS 7 BP 685 EP 695 PG 11 WC Chemistry, Medicinal SC Pharmacology & Pharmacy GA CD6KM UT WOS:000351198000010 PM 25751268 ER PT J AU Connelly, SJ Wiedner, ES Appel, AM AF Connelly, Samantha J. Wiedner, Eric S. Appel, Aaron M. TI Predicting the reactivity of hydride donors in water: thermodynamic constants for hydrogen SO DALTON TRANSACTIONS LA English DT Article ID TRANSITION-METAL-COMPLEXES; ELECTRODE-POTENTIALS; CARBON-DIOXIDE; AQUEOUS-SOLUTION; CO2 REDUCTION; HYDRATION ENERGIES; NICKEL-CATALYST; ACIDITY; PROTON; H-2 AB The chemical reactivity of hydride complexes can be predicted using bond strengths for homolytic and heterolytic cleavage of bonds to hydrogen. To determine these bond strengths, thermodynamic constants describing the stability of H+, H-center dot, H-, and H-2 are essential and need to be used uniformly to enable the prediction of reactivity and equilibria. Due to discrepancies in the literature for the constants used in water, we propose the use of a set of self-consistent constants with convenient standard states. C1 [Connelly, Samantha J.; Wiedner, Eric S.; Appel, Aaron M.] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Wiedner, ES (reprint author), Pacific NW Natl Lab, PBO 999,MS K2-57, Richland, WA 99352 USA. EM eric.wiedner@pnnl.gov; aaron.appel@pnnl.gov OI Wiedner, Eric/0000-0002-7202-9676; Appel, Aaron/0000-0002-5604-1253 FU U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences Biosciences FX The authors thank Dr James Muckerman, Dr Daniel DuBois, Dr Donald Camaioni, and Prof. Alexander Miller for helpful discussions. The work was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences & Biosciences. NR 63 TC 17 Z9 17 U1 7 U2 23 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1477-9226 EI 1477-9234 J9 DALTON T JI Dalton Trans. PY 2015 VL 44 IS 13 BP 5933 EP 5938 DI 10.1039/c4dt03841j PG 6 WC Chemistry, Inorganic & Nuclear SC Chemistry GA CE0EF UT WOS:000351476600001 PM 25697077 ER PT J AU Shamloo, A Heibatollahi, M Mofrad, MRK AF Shamloo, Amir Heibatollahi, Motahare Mofrad, Mohammad R. K. TI Directional migration and differentiation of neural stem cells within three-dimensional microenvironments SO INTEGRATIVE BIOLOGY LA English DT Article ID TRAUMATIC BRAIN-INJURY; EXTRACELLULAR-MATRIX; MICROFLUIDIC DEVICE; PRECURSOR CELLS; GROWTH-FACTOR; SUBVENTRICULAR ZONE; ADULT NEUROGENESIS; CHEMOTAXIS; NEURONS; REPAIR AB A Harnessing neural stem cells to repair neuronal damage is a promising potential treatment for neuronal diseases. To enable future therapeutic efficacy, the survival, proliferation, migration and differentiation of neural stem/progenitor cells (NPCs) should be accurately studied and optimized in in vitro platforms before transplanting these cells into the body for treatment purposes. Such studies can determine the appropriate quantities of the biochemical and biomechanical factors needed to control and optimize NPC behavior in vivo. In this study, NPCs were cultured within a microfluidic device while being encapsulated within the collagen matrix. The migration and differentiation of NPCs were studied in response to varying concentrations of nerve growth factor (NGF) and within varying densities of collagen matrices. It was shown that the migration and differentiation of NPCs can be significantly improved by providing the appropriate range of NGF concentrations while encapsulating the cells within the collagen matrix of optimal density. In particular, it was observed that within collagen matrices of intermediate density (0.9 mg ml(-1)), NPCs have a higher ability to migrate farther and in a collective manner while their differentiation into neurons is significantly higher and the cells can form protrusions and connections with their neighboring cells. Within collagen matrices with higher densities (1.8 mg ml (-1)), the cells did not migrate significantly as compared to the ones within lower matrix densities; within the matrices with lower collagen densities (0.45 mg ml(-1)) most of the cells migrated in an individual manner. However, no significant differentiation into neurons was observed for these two cases. It was also found that depending on the collagen matrix density, a minimum concentration of NGF caused a collective migration of NPCs, and a minimum concentration gradient of this factor stimulated the directional navigation of the cells. The results of this study can be implemented in designing platforms appropriate for regeneration of damaged neuronal systems. C1 [Shamloo, Amir; Heibatollahi, Motahare; Mofrad, Mohammad R. K.] Univ Calif Berkeley, Dept Bioengn, Mol Cell Biomech Lab, Berkeley, CA 94720 USA. [Shamloo, Amir; Heibatollahi, Motahare; Mofrad, Mohammad R. K.] Univ Calif Berkeley, Dept Mech Engn, Mol Cell Biomech Lab, Berkeley, CA 94720 USA. [Shamloo, Amir] Sharif Univ Technol, Dept Mech Engn, Tehran, Iran. [Mofrad, Mohammad R. K.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Phys Biosci Div, Berkeley, CA 94720 USA. RP Mofrad, MRK (reprint author), Univ Calif Berkeley, Dept Bioengn, Mol Cell Biomech Lab, Berkeley, CA 94720 USA. EM mofrad@berkeley.edu FU National Science Foundation CAREER award [CBET-0955291]; Siebel Stem Cell Institute FX Financial support through a National Science Foundation CAREER award CBET-0955291 (M.R.K.M.) and a Siebel Stem Cell Institute post-doctoral fellowship (A.S.) is gratefully acknowledged. The authors would also like to thank the UC Berkeley Stem Cell Center and QB3 Shared Stem Cell Facilities for their assistance throughout this project. Fruitful discussions with Dr David Schaffer and the members of the Molecular Cell Biomechanics Laboratory are highly appreciated. NR 60 TC 5 Z9 6 U1 3 U2 27 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1757-9694 EI 1757-9708 J9 INTEGR BIOL-UK JI Integr. Biol. PY 2015 VL 7 IS 3 BP 335 EP 344 DI 10.1039/c4ib00144c PG 10 WC Cell Biology SC Cell Biology GA CD5OA UT WOS:000351136500006 PM 25633746 ER PT J AU Williams, AP Seager, R Macalady, AK Berkelhammer, M Crimmins, MA Swetnam, TW Trugman, AT Buenning, N Noone, D McDowell, NG Hryniw, N Mora, CI Rahn, T AF Williams, A. Park Seager, Richard Macalady, Alison K. Berkelhammer, Max Crimmins, Michael A. Swetnam, Thomas W. Trugman, Anna T. Buenning, Nikolaus Noone, David McDowell, Nate G. Hryniw, Natalia Mora, Claudia I. Rahn, Thom TI Correlations between components of the water balance and burned area reveal new insights for predicting forest fire area in the southwest United States SO INTERNATIONAL JOURNAL OF WILDLAND FIRE LA English DT Article DE fire danger; tree mortality; warming ID CLIMATE-CHANGE; NORTH-AMERICA; WESTERN USA; WILDFIRE; DROUGHT; WIND; TEMPERATURE; PERSPECTIVE; VARIABILITY; SENSITIVITY AB We related measurements of annual burned area in the southwest United States during 1984-2013 to records of climate variability. Within forests, annual burned area correlated at least as strongly with spring-summer vapour pressure deficit (VPD) as with 14 other drought-related metrics, including more complex metrics that explicitly represent fuel moisture. Particularly strong correlations with VPD arise partly because this term dictates the atmospheric moisture demand. Additionally, VPD responds to moisture supply, which is difficult to measure and model regionally due to complex micrometeorology, land cover and terrain. Thus, VPD appears to be a simple and holistic indicator of regional water balance. Coupled with the well-known positive influence of prior-year cold season precipitation on fuel availability and connectivity, VPD may be utilised for burned area forecasts and also to infer future trends, though these are subject to other complicating factors such as land cover change and management. Assuming an aggressive greenhouse gas emissions scenario, climate models predict mean spring-summer VPD will exceed the highest recorded values in the southwest in nearly 40% of years by the middle of this century. These results forewarn of continued increases in burned forest area in the southwest United States, and likely elsewhere, when fuels are not limiting. C1 [Williams, A. Park; Seager, Richard] Columbia Univ, Lamont Doherty Earth Observ, Palisades, NY 10964 USA. [Macalady, Alison K.; Swetnam, Thomas W.] Univ Arizona, Tree Ring Res Lab, Tucson, AZ 85724 USA. [Berkelhammer, Max; Noone, David] Univ Colorado, Cooperat Inst Res Environm Sci, Dept Atmospher & Ocean Sci, Boulder, CO 80309 USA. [Crimmins, Michael A.] Univ Arizona, Dept Soil Water & Environm Sci, Tucson, AZ 85721 USA. [Trugman, Anna T.] Princeton Univ, Dept Atmospher & Ocean Sci, Princeton, NJ 08544 USA. [Buenning, Nikolaus] Univ So Calif, Dept Earth Sci, Los Angeles, CA 90089 USA. [McDowell, Nate G.; Mora, Claudia I.; Rahn, Thom] Los Alamos Natl Lab, Div Earth & Environm Sci, Los Alamos, NM 87545 USA. [Hryniw, Natalia] Univ Washington, Dept Atmospher Sci, Seattle, WA 98195 USA. RP Williams, AP (reprint author), Columbia Univ, Lamont Doherty Earth Observ, Palisades, NY 10964 USA. EM williams@ldeo.columbia.edu RI Williams, Park/B-8214-2016; Mora, Claudia/B-5511-2017; OI Williams, Park/0000-0001-8176-8166; Mora, Claudia/0000-0003-2042-0208; Rahn, Thomas/0000-0001-8634-1348 FU LANL-LDRD; DoE-BER; NOAA [NA10OAR4310137]; NSF FX This work was supported by LANL-LDRD and DoE-BER. RS was supported by NOAA awards NA10OAR4310137 (Global Decadal Hydroclimate Variability and Change) and NSF award EASM2: Linking Near-term Future Changes in Weather and Hydroclimate in Western North America to Adaptation for Ecosystem and Water Management. Thanks to J. T. Abatzoglou, C. D. Allen, C. Baisan, B. I. Cook, E. R. Cook, C. Daly, E. H.(T.) Hogg, B. E. Law, R. R. Linn, N. Pederson, S. A. Rauscher, J. Sheffield, and A. M. Strong for insightful conversations. NR 76 TC 19 Z9 19 U1 7 U2 35 PU CSIRO PUBLISHING PI CLAYTON PA UNIPARK, BLDG 1, LEVEL 1, 195 WELLINGTON RD, LOCKED BAG 10, CLAYTON, VIC 3168, AUSTRALIA SN 1049-8001 EI 1448-5516 J9 INT J WILDLAND FIRE JI Int. J. Wildland Fire PY 2015 VL 24 IS 1 BP 14 EP 26 DI 10.1071/WF14023 PG 13 WC Forestry SC Forestry GA CD9TV UT WOS:000351442300002 ER PT J AU Zhang, PF Jiang, XG Wan, S Dai, S AF Zhang, Pengfei Jiang, Xueguang Wan, Shun Dai, Sheng TI Advancing polymers of intrinsic microporosity by mechanochemistry SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID COVALENT ORGANIC FRAMEWORKS; SOLVENT-FREE SYNTHESIS; POROUS POLYMERS; 1,4-DICYANOTETRAFLUOROBENZENE; POLYCONDENSATION; CATALYSIS; ZEOLITES; DESIGN; PIMS AB Herein, we report a fast (15 min) and solvent-free mechanochemical approach to construct polymers of intrinsic microporosity (PIMs) with high molecular mass and low polydispersity by solid grinding. The enhanced reaction efficiency results from the instantaneous frictional heating and continuous exposure of active sites within those solid reactants. C1 [Zhang, Pengfei; Wan, Shun; Dai, Sheng] Oak Ridge Natl Lab, Chem Sci Div, Oak Ridge, TN 37831 USA. [Jiang, Xueguang; Dai, Sheng] Univ Tennessee, Dept Chem, Knoxville, TN 37996 USA. RP Zhang, PF (reprint author), Oak Ridge Natl Lab, Chem Sci Div, Oak Ridge, TN 37831 USA. EM chemistryzpf@163.com; dais@ornl.gov RI Jiang, Xueguang/J-5784-2013; Dai, Sheng/K-8411-2015; Zhang, Pengfei/I-5484-2013 OI Jiang, Xueguang/0000-0002-9937-6029; Dai, Sheng/0000-0002-8046-3931; FU Fluid Interface Reactions, Structures and Transport (FIRST) Center, an Energy Frontier Research Center - US Department of Energy, Office of Science, Office of Basic Energy Sciences FX This work was supported as part of the Fluid Interface Reactions, Structures and Transport (FIRST) Center, an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Office of Basic Energy Sciences. NR 27 TC 5 Z9 5 U1 6 U2 51 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7488 EI 2050-7496 J9 J MATER CHEM A JI J. Mater. Chem. A PY 2015 VL 3 IS 13 BP 6739 EP 6741 DI 10.1039/c4ta07196d PG 3 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA CE1DM UT WOS:000351552300003 ER PT J AU Hansson, R Ericsson, LKE Holmes, NP Rysz, J Opitz, A Campoy-Quiles, M Wang, EG Barr, MG Kilcoyne, ALD Zhou, XJ Dastoor, P Moons, E AF Hansson, Rickard Ericsson, Leif K. E. Holmes, Natalie P. Rysz, Jakub Opitz, Andreas Campoy-Quiles, Mariano Wang, Ergang Barr, Matthew G. Kilcoyne, A. L. David Zhou, Xiaojing Dastoor, Paul Moons, Ellen TI Vertical and lateral morphology effects on solar cell performance for a thiophene-quinoxaline copolymer: PC70BM blend SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID RAY-ABSORPTION SPECTROSCOPY; ELECTRON-ESCAPE DEPTH; COATED THIN-FILMS; PHASE-SEPARATION; PHOTOVOLTAIC DEVICES; PROCESSING ADDITIVES; NANOSCALE MORPHOLOGY; ACTIVE LAYERS; POLYMER-BLEND; EFFICIENCY AB The distribution of electron donor and acceptor in the active layer is known to strongly influence the electrical performance of polymer solar cells for most of the high performance polymer: fullerene systems. The formulation of the solution from which the active layer is spincoated plays an important role in the quest for morphology control. We have studied how the choice of solvent and the use of small amounts of a low vapour pressure additive in the coating solution influence the film morphology and the solar cell performance for blends of poly[2,3-bis-(3-octyloxyphenyl) quinoxaline-5,8-diyl-altthiophene-2,5-diyl] (TQ1) and [6,6]-phenyl C-71-butyric acid methyl ester (PC70BM). We have investigated the lateral morphology using atomic force microscopy (AFM) and scanning transmission X-ray microscopy (STXM), the vertical morphology using dynamic secondary ion mass spectrometry (d-SIMS) and variable-angle spectroscopic ellipsometry (VASE), and the surface composition using near-edge X-ray absorption fine structure (NEXAFS). The lateral phase-separated domains observed in films spincoated from single solvents, increase in size with increasing solvent vapour pressure and decreasing PC70BM solubility, but are not observed when 1-chloronaphthalene (CN) is added. A strongly TQ1-enriched surface layer is formed in all TQ1: PC70BM blend films and rationalized by surface energy differences. The photocurrent and power conversion efficiency strongly increased upon the addition of CN, while the leakage current decreased by one to two orders of magnitude. The higher photocurrent correlates with the finer lateral structure and stronger TQ1-enrichment at the interface with the electron-collecting electrode. This indicates that the charge transport and collection are not hindered by this polymer-enriched surface layer. Neither the open-circuit voltage nor the series resistance of the devices are sensitive to the differences in morphology. C1 [Hansson, Rickard; Ericsson, Leif K. E.; Moons, Ellen] Karlstad Univ, Dept Engn & Phys, S-65188 Karlstad, Sweden. [Holmes, Natalie P.; Barr, Matthew G.; Zhou, Xiaojing; Dastoor, Paul] Univ Newcastle, Ctr Organ Elect, Callaghan, NSW 2308, Australia. [Rysz, Jakub] Jagiellonian Univ, Inst Phys, PL-30059 Krakow, Poland. [Opitz, Andreas] Humboldt Univ, Dept Phys, D-12489 Berlin, Germany. [Campoy-Quiles, Mariano] Inst Ciencia Mat Barcelona ICMAB CSIC, Bellaterra 08193, Spain. [Wang, Ergang] Chalmers Univ Technol, Dept Chem & Chem Engn, S-41296 Gothenburg, Sweden. [Kilcoyne, A. L. David] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. RP Moons, E (reprint author), Karlstad Univ, Dept Engn & Phys, S-65188 Karlstad, Sweden. EM ellen.moons@kau.se RI Opitz, Andreas/L-7700-2015; Moons, Ellen/B-6252-2011; Rysz, Jakub/F-1043-2012; Kilcoyne, David/I-1465-2013; Wang, Ergang/F-8157-2010; Campoy-Quiles, Mariano/A-7768-2013 OI Opitz, Andreas/0000-0002-3214-8398; Moons, Ellen/0000-0002-1609-8909; Rysz, Jakub/0000-0003-1668-3398; Wang, Ergang/0000-0002-4942-3771; Campoy-Quiles, Mariano/0000-0002-8911-640X FU Swedish Research Council [2010-4155]; Goran Gustafsson Foundation for Research in Natural Sciences and Medicine; Spanish Ministerio de Economia y Competitividad [MAT2012-37776]; Rontgen-Angstrom-Cluster; Swedish Research Council; Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231] FX The authors thank Ana Sofia Anselmo and Monika Josiek for valuable experimental contributions in the initial stages of the research project, Christian Muller for the ellipsometry experiment and Alexei Preobrajenski at beamline D1011, MAX-IV Laboratory, for valuable technical advice with the NEXAFS experiments. E.M. acknowledges funding from the Swedish Research Council (Project 2010-4155) and the Goran Gustafsson Foundation for Research in Natural Sciences and Medicine. M.C.-Q. thanks the Spanish Ministerio de Economia y Competitividad for financial support through project PHOTOCOMB (MAT2012-37776). A.O. acknowledges the Rontgen-Angstrom-Cluster for financial support. E.W. acknowledges the Swedish Research Council for financial support. This work was performed in part at the Materials node of the Australian National Fabrication Facility, which is a company established under the National Collaborative Research Infrastructure Strategy to provide nano and microfabrication facilities for Australia's researchers. STXM data were acquired at beamline 5.3.2.2 at the Advanced Light Source, Berkeley, 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 61 TC 11 Z9 11 U1 4 U2 29 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7488 EI 2050-7496 J9 J MATER CHEM A JI J. Mater. Chem. A PY 2015 VL 3 IS 13 BP 6970 EP 6979 DI 10.1039/c5ta00683j PG 10 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA CE1DM UT WOS:000351552300034 ER PT J AU Xin, FX Wang, XL Bai, JM Wen, W Tian, HJ Wang, CS Han, WQ AF Xin, Fengxia Wang, Xiaoliang Bai, Jianming Wen, Wen Tian, Huajun Wang, Chunsheng Han, Weiqiang TI A lithiation/delithiation mechanism of monodispersed MSn5 (M = Fe, Co and FeCo) nanospheres SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID LITHIUM-ION BATTERIES; ANODE MATERIAL; HIGH-CAPACITY; ELECTROCHEMICAL PROPERTIES; SECONDARY BATTERIES; SN NANOCRYSTALS; LI; PERFORMANCE; STORAGE; ALLOY AB A designed Sn based alloy host as a higher capacity and longer cycle life next generation lithium-ion battery, consisting of monodisperse nanospheres of intermetallic MSn5 (M = Fe, Co and FeCo) phases was synthesized by a nanocrystal conversion chemistry method using preformed Sn nanospheres as templates. The same crystal structure, identical particle surface morphology and the similar particle size distribution (30-50 nm) of these intermetallic MSn5 (M = Fe, Co and FeCo) phases are ideal for comparison of the electrochemical performance, reaction mechanism, thermodynamics and kinetics during lithiation/delithiation. Importantly, MSn5 (M = Fe, Co and FeCo) phases with defect structures Fe0.74Sn5, Co0.83Sn5 and Fe0.35Co0.35Sn5, exhibit the highest theoretical capacity of >917 mA h g(-1) among the reported M-Sn (M is electro-chemically inactive) based intermetallic anodes. The ex situ XRD and XAFS illustrate the complete reversibility of MSn5 (M = Fe, Co and FeCo) phases during lithium insertion/extraction for the first cycle. The Fe0.35Co0.35Sn5 anode can take advantage of both high capacity of Fe0.74Sn5 and long cycle life of Co0.83Sn5, providing 736 mA h g(-1) and maintaining 92.7% of initial capacity after 100 cycles with an average capacity loss of only 0.07% per cycle. The excellent electrochemical performance of the Fe0.5Co0.5Sn5 system is attributed to higher reversibility, lower reaction resistance. This work provides a novel insight toward designing and exploring an optimal Sn based alloy anode for next generation Li-ion batteries. C1 [Xin, Fengxia; Wang, Xiaoliang; Tian, Huajun; Han, Weiqiang] Chinese Acad Sci, Ningbo Inst Mat Technol & Engn, Ningbo 315201, Zhejiang, Peoples R China. [Bai, Jianming] Brookhaven Natl Lab, Natl Synchrotron Light Source, Upton, NY 11973 USA. [Wen, Wen] Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China. [Wang, Chunsheng] Univ Maryland, Dept Chem & Biomol Engn, College Pk, MD 20742 USA. RP Han, WQ (reprint author), Chinese Acad Sci, Ningbo Inst Mat Technol & Engn, Ningbo 315201, Zhejiang, Peoples R China. EM cswang@umd.edu; hanweiqiang@nimte.ac.cn RI Tian, Huajun/E-8816-2011; Han, WQ/E-2818-2013; Wang, Chunsheng/H-5767-2011; Bai, Jianming/O-5005-2015 OI Wang, Chunsheng/0000-0002-8626-6381; FU Chinese Project Academy of Science [XDA01020304]; National Natural Science Foundation of China [51371186]; Ningbo 3315 International Team of Advanced Energy Storage Materials; Zhejiang Province Key Science and Technology Innovation Team [2013PT16]; China Postdoctoral Science Foundation [2013M541807]; Ningbo Natural Science Foundation [2014A610046] FX This work is supported by the "Strategic Priority Research Program" of the Chinese Project Academy of Science, Grant no. XDA01020304, the National Natural Science Foundation of China (Grant no. 51371186), Ningbo 3315 International Team of Advanced Energy Storage Materials, Zhejiang Province Key Science and Technology Innovation Team (Grant no. 2013PT16), China Postdoctoral Science Foundation funded project (Grant no. 2013M541807) and Ningbo Natural Science Foundation (Grant no. 2014A610046). NR 48 TC 8 Z9 8 U1 11 U2 65 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7488 EI 2050-7496 J9 J MATER CHEM A JI J. Mater. Chem. A PY 2015 VL 3 IS 13 BP 7170 EP 7178 DI 10.1039/c4ta06960a PG 9 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA CE1DM UT WOS:000351552300057 ER PT J AU Li, Z Gosztola, DJ Sun, CJ Heald, SM Sun, YG AF Li, Zheng Gosztola, David J. Sun, Cheng-Jun Heald, Steve M. Sun, Yugang TI Exceptional enhancement of Raman scattering on silver chlorobromide nanocube photonic crystals: chemical and photonic contributions SO JOURNAL OF MATERIALS CHEMISTRY C LA English DT Article ID SINGLE-MOLECULE DETECTION; OPTICAL-PROPERTIES; SPECTROSCOPY; SERS; SPECTRA; NANOPARTICLES; ELECTRODE; PYRIDINE; NANOSTRUCTURES; IDENTIFICATION AB Photonic crystals made from self-assembly of mono-dispersed AgClxBr1-x nanocubes, which are not plasmonically active, have been discovered to exceptionally enhance the Raman scattering of molecules chemically adsorbed on their surfaces. Comprehensive control measurements and X-ray absorption near-edge structure spectroscopy indicate that the Raman enhancement on AgClxBr1-x nanocube photonic crystals is primarily ascribed to the chemical enhancement mechanism associated with the chemical interactions between adsorbing molecules and the AgClxBr1-x surfaces. In addition, the ordering of AgClxBr1-x nanocubes in the photonic crystals can selectively reflect Raman scattering back to the detector at the bandgap position of the photonic crystals to provide additional enhancement, i.e., photonic mode enhancement. The thiophenol molecules adsorbed on AgCl0.44Br0.56 nanocube photonic crystals exhibit astonishingly strong Raman signals that are on the same order of magnitude as those recorded from the thiophenol molecules adsorbed on the assembled Ag nanocubes. C1 [Li, Zheng; Gosztola, David J.; Sun, Yugang] Argonne Natl Lab, Ctr Nanoscale Mat, Argonne, IL 60439 USA. [Sun, Cheng-Jun; Heald, Steve M.] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA. RP Sun, YG (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; Gosztola, David/D-9320-2011; Li, Zheng/L-1355-2016 OI Sun, Yugang /0000-0001-6351-6977; Gosztola, David/0000-0003-2674-1379; Li, Zheng/0000-0001-5281-8101 FU U. S. Department of Energy, Office of Science, Office of Basic Energy Sciences User Facility [DE-AC02-06CH11357]; US Department of Energy - Basic Energy Sciences; Canadian Light Source; University of Washington; Advanced Photon Source; U. S. DOE [DE-AC02-06CH11357] FX This work was performed 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. PNC/XSD facilities at the Advanced Photon Source, and research at these facilities, are supported by the US Department of Energy - Basic Energy Sciences, the Canadian Light Source and its funding partners, the University of Washington, and the Advanced Photon Source. Use of the Advanced Photon Source, an Office of Science User Facility operated for the U. S. Department of Energy (DOE) Office of Science by Argonne National Laboratory, was supported by the U. S. DOE under Contract no. DE-AC02-06CH11357. NR 47 TC 1 Z9 1 U1 1 U2 24 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7526 EI 2050-7534 J9 J MATER CHEM C JI J. Mater. Chem. C PY 2015 VL 3 IS 11 BP 2455 EP 2461 DI 10.1039/c5tc00077g PG 7 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA CD3NA UT WOS:000350984200003 ER PT J AU Park, M Jung, SH Lim, J Kim, DY Kim, HJ Lee, S Jung, H Lee, S Lee, C Lee, JK AF Park, Myeongjin Jung, Seok-Heon Lim, Jaehoon Kim, Dae-Young Kim, Hee-Jin Lee, Seungyong Jung, Heeyoung Lee, Seonghoon Lee, Changhee Lee, Jin-Kyun TI Semiconductor nanocrystals in fluorous liquids for the construction of light-emitting diodes SO JOURNAL OF MATERIALS CHEMISTRY C LA English DT Article ID QUANTUM DOTS; ORGANIC ELECTRONICS; POLYMER; DEVICES; ELECTROLUMINESCENCE; HYDROFLUOROETHERS; SEPARATION; EFFICIENCY; SOLVENTS; BRIGHT AB This communication reports a materials handling strategy based on fluorous materials chemistry using CdSe/CdS/CdZnS core-shell type semiconductor nanocrystals. When the crystals were treated with the semi-perfluoroalkanethiol ligands in the presence of (Pr2EtN)-Pr-i, the surface-modified nanocrystals (R(F)1-NC and R(F)2-NC) became soluble in the fluorous liquids. Solutions of R(F)1-NC and R(F)2-NC in HFE-7500 enabled the solution-casting of nanocrystalline films on top of a small-molecular hole-transporting layer and provided layered structures suitable for light-emitting diode fabrication. C1 [Park, Myeongjin; Jung, Heeyoung; Lee, Changhee] Seoul Natl Univ, Dept Elect & Comp Engn, Interuniv Semicond Res Ctr, Seoul 151744, South Korea. [Jung, Seok-Heon; Kim, Dae-Young; Kim, Hee-Jin; Lee, Seungyong; Lee, Jin-Kyun] Inha Univ, Dept Polymer Sci & Engn, Inchon 402751, South Korea. [Lim, Jaehoon] Los Alamos Natl Lab, Div Chem, Los Alamos, NM 87545 USA. [Lee, Seonghoon] Seoul Natl Univ, Sch Chem, Seoul 151747, South Korea. RP Lee, C (reprint author), Seoul Natl Univ, Dept Elect & Comp Engn, Interuniv Semicond Res Ctr, Seoul 151744, South Korea. EM chlee7@snu.ac.kr; jkl36@inha.ac.kr RI Lee, Changhee/A-2471-2009 OI Lee, Changhee/0000-0003-2800-8250 FU Fundamental R&D Program for Core Technology of Materials [10041220]; Industrial Strategic Technology Development Program - Ministry of Trade, Industry and Energy (MOTIE, Korea) [10045145]; Inha University FX This study was supported by the Fundamental R&D Program for Core Technology of Materials (grant no. 10041220) and Industrial Strategic Technology Development Program (grant no. 10045145) funded by the Ministry of Trade, Industry and Energy (MOTIE, Korea). J.K.L. thanks Inha University for partial support. NR 35 TC 1 Z9 1 U1 1 U2 13 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7526 EI 2050-7534 J9 J MATER CHEM C JI J. Mater. Chem. C PY 2015 VL 3 IS 12 BP 2759 EP 2762 DI 10.1039/c4tc02503b PG 4 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA CD9YZ UT WOS:000351459300006 ER PT J AU Kim, KJ Chong, XY Kreider, PB Ma, GH Ohodnicki, PR Baltrus, JP Wang, AX Chang, CH AF Kim, Ki-Joong Chong, Xinyuan Kreider, Peter B. Ma, Guoheng Ohodnicki, Paul R. Baltrus, John P. Wang, Alan X. Chang, Chih-Hung TI Plasmonics-enhanced metal-organic framework nanoporous films for highly sensitive near-infrared absorption SO JOURNAL OF MATERIALS CHEMISTRY C LA English DT Article ID THIN-FILMS; SENSING APPLICATIONS; RAMAN-SPECTROSCOPY; GAS; FABRICATION; SENSORS; NANOCRYSTALS; NANOANTENNAS; ADSORPTION; ELECTRODES AB Combined plasmonic nanocrystals and metal-organic framework thin-films are fabricated for sensing gases in the near-infrared range. This nanocomposite thin-film shows a highly sensitive response in near-infrared absorption, which is attributed to preconcentration of gas molecules in metal-organic framework pores causing close proximity to the electromagnetic fields at the plasmonic nanocrystal surface. C1 [Kim, Ki-Joong; Kreider, Peter B.; Ma, Guoheng; Chang, Chih-Hung] Oregon State Univ, Sch Chem, Biol Environm Engn, Corvallis, OR 97331 USA. [Chong, Xinyuan; Wang, Alan X.] Oregon State Univ, Sch Elect Engn & Comp Sci, Corvallis, OR 97331 USA. [Ohodnicki, Paul R.; Baltrus, John P.] US DOE, Natl Energy Technol Lab, Pittsburgh, PA 15236 USA. RP Chang, CH (reprint author), Oregon State Univ, Sch Chem, Biol Environm Engn, Corvallis, OR 97331 USA. EM wang@eecs.oregonstate.edu; chih-hung.chang@oregonstate.edu NR 52 TC 8 Z9 8 U1 4 U2 44 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7526 EI 2050-7534 J9 J MATER CHEM C JI J. Mater. Chem. C PY 2015 VL 3 IS 12 BP 2763 EP 2767 DI 10.1039/c4tc02846e PG 5 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA CD9YZ UT WOS:000351459300007 ER PT J AU Benk, MP Miyakawa, RH Chao, W Wang, YG Wojdyla, A Johnson, DG Donoghue, AP Goldberg, KA AF Benk, Markus P. Miyakawa, Ryan H. Chao, Weilun Wang, Yow-Gwo Wojdyla, Antoine Johnson, David G. Donoghue, Alexander P. Goldberg, Kenneth A. TI Broader view on extreme ultraviolet masks: adding complementary imaging modes to the SHARP microscope SO JOURNAL OF MICRO-NANOLITHOGRAPHY MEMS AND MOEMS LA English DT Article DE photomask; extreme ultraviolet; mask imaging; zoneplate; Zernike phase contrast; differential interference contrast ID X-RAY MICROSCOPY; PHASE-CONTRAST; ZONE PLATES AB The authors are expanding the capabilities of the SHARP microscope by implementing complementary imaging modes. SHARP (the SEMATECH High-NA Actinic Reticle Review Project) is an actinic, synchrotron-based microscope dedicated to extreme ultraviolet photomask research. SHARP's programmable Fourier synthesis illuminator and its use of Fresnel zoneplate lenses as imaging optics provide a versatile framework, facilitating the implementation of diverse modes beyond conventional imaging. In addition to SHARP's set of standard zoneplates, we have created more than 100 zoneplates for complementary imaging modes, all designed to extract additional information from photomasks, to improve navigation, and to enhance defect detection. More than 50 new zoneplates are installed in the tool; the remaining lenses are currently in production. We discuss the design and fabrication of zoneplates for complementary imaging modes and present image data, obtained using Zernike phase contrast and different implementations of differential interference contrast (DIC). First results show that Zernike phase contrast can significantly increase the signal from phase defects in SHARP image data, thus improving the sensitivity of the microscope. DIC is effective on a variety of features, including phase defects and intensity speckle from substrate and multilayer roughness. The additional imaging modes are now available to users of the SHARP microscope. (C) The Authors. C1 [Benk, Markus P.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, SHARP Microscope, Ctr Xray Opt, Berkeley, CA 94720 USA. [Miyakawa, Ryan H.; Wojdyla, Antoine; Johnson, David G.; Donoghue, Alexander P.; Goldberg, Kenneth A.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Ctr Xray Opt, Berkeley, CA 94720 USA. [Chao, Weilun; Wang, Yow-Gwo] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Wang, Yow-Gwo] Univ Calif Berkeley, Dept EECS, Berkeley, CA 94720 USA. RP Benk, MP (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, SHARP Microscope, Ctr Xray Opt, 1 Cyclotron Rd, Berkeley, CA 94720 USA. EM mpbenk@lbl.gov FU Office of Science, Office of Basic Energy Sciences, of U.S. Department of Energy [DE-AC02-05CH11231]; SEMATECH FX The Advanced Light Source at Lawrence Berkeley National Laboratory is supported by the Director, Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. We gratefully acknowledge SEMATECH funding of the SHARP microscope, and Anne Rudack the SHARP project manager. Test masks used in imaging experiments described above were provided by GLOBALFOUNDRIES and Intel. NR 16 TC 2 Z9 2 U1 1 U2 2 PU SPIE-SOC PHOTO-OPTICAL INSTRUMENTATION ENGINEERS PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98225 USA SN 1932-5150 EI 1932-5134 J9 J MICRO-NANOLITH MEM JI J. Micro-Nanolithogr. MEMS MOEMS PD JAN PY 2015 VL 14 IS 1 AR 013507 DI 10.1117/1.JMM.14.1.013507 PG 8 WC Engineering, Electrical & Electronic; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Optics SC Engineering; Science & Technology - Other Topics; Materials Science; Optics GA CE2IZ UT WOS:000351640600015 ER PT J AU Imam, S Noguera, DR Donohue, TJ AF Imam, Saheed Noguera, Daniel R. Donohue, Timothy J. TI CceR and AkgR Regulate Central Carbon and Energy Metabolism in Alphaproteobacteria SO MBIO LA English DT Article ID RHODOBACTER-SPHAEROIDES; ESCHERICHIA-COLI; BACILLUS-SUBTILIS; CATABOLITE REPRESSION; MICROBIAL-METABOLISM; GLUCOSE-METABOLISM; GENE-EXPRESSION; BINDING-SITE; PROTEIN; IDENTIFICATION AB Many pathways of carbon and energy metabolism are conserved across the phylogeny, but the networks that regulate their expression or activity often vary considerably among organisms. In this work, we show that two previously uncharacterized transcription factors (TFs) are direct regulators of genes encoding enzymes of central carbon and energy metabolism in the alphaproteobacterium Rhodobacter sphaeroides. The LacI family member CceR (RSP_1663) directly represses genes encoding enzymes in the Entner-Doudoroff pathway, while activating those encoding the F1F0 ATPase and enzymes of the tricarboxylic acid (TCA) cycle and gluconeogenesis, providing a direct transcriptional network connection between carbon and energy metabolism. We identified bases that are important for CceR DNA binding and showed that DNA binding by this TF is inhibited by 6-phosphogluconate. We also showed that the GntR family TF AkgR (RSP_0981) directly activates genes encoding several TCA cycle enzymes, and we identified conditions where its activity is increased. The properties of single and double Delta CceR and Delta AkgR mutants illustrate that these 2 TFs cooperatively regulate carbon and energy metabolism. Comparative genomic analysis indicates that CceR and AkgR orthologs are found in other alphaproteobacteria, where they are predicted to have a conserved function in regulating central carbon metabolism. Our characterization of CceR and AkgR has provided important new insight into the networks that control central carbon and energy metabolism in alphaproteobacteria that can be exploited to modify or engineer new traits in these widespread and versatile bacteria. IMPORTANCE To extract and conserve energy from nutrients, cells coordinate a set of metabolic pathways into integrated networks. Many pathways that conserve energy or interconvert metabolites are conserved across cells, but the networks regulating these processes are often highly variable. In this study, we characterize two previously unknown transcriptional regulators of carbon and energy metabolism that are conserved in alphaproteobacteria, a group of abundant, environmentally and biotechnologically important organisms. We identify the genes they regulate, the DNA sequences they recognize, the metabolite that controls the activity of one of the regulators, and conditions where they are required for growth. We provide important new insight into conserved cellular networks that can also be used to improve a variety of hosts for converting feedstock into valuable products. C1 [Imam, Saheed] Univ Wisconsin, Grad Program Cellular & Mol Biol, Madison, WI 53706 USA. [Imam, Saheed; Donohue, Timothy J.] Univ Wisconsin, Dept Bacteriol, Madison, WI 53706 USA. [Imam, Saheed; Noguera, Daniel R.; Donohue, Timothy J.] Univ Wisconsin, DOE Great Lakes Bioenergy Res Ctr, Madison, WI 53706 USA. [Noguera, Daniel R.] Univ Wisconsin, Dept Civil & Environm Engn, Madison, WI 53706 USA. RP Donohue, TJ (reprint author), Univ Wisconsin, Dept Bacteriol, Madison, WI 53706 USA. EM tdonohue@bact.wisc.edu OI Donohue, Timothy/0000-0001-8738-2467 FU Department of Energy, Office of Science, Great Lakes Bioenergy Research Center [DE-FC02-07ER64494]; Genomics: GTL and SciDAC programs [DE-FG02-04ER25627]; University of Wisconsin-Madison Bacteriology Department FX This work was supported by the Department of Energy, Office of Science, Great Lakes Bioenergy Research Center (DE-FC02-07ER64494), the Genomics: GTL and SciDAC programs (DE-FG02-04ER25627), and a William H. Peterson Predoctoral Fellowship from the University of Wisconsin-Madison Bacteriology Department to S.I. NR 65 TC 3 Z9 3 U1 1 U2 8 PU AMER SOC MICROBIOLOGY PI WASHINGTON PA 1752 N ST NW, WASHINGTON, DC 20036-2904 USA SN 2150-7511 J9 MBIO JI mBio PD JAN-FEB PY 2015 VL 6 IS 1 AR e02461-14 DI 10.1128/mBio.02461-14 PG 15 WC Microbiology SC Microbiology GA CC8PZ UT WOS:000350631900034 ER PT J AU Kim, HK Falugi, F Thomer, L Missiakas, DM Schneewind, O AF Kim, Hwan Keun Falugi, Fabiana Thomer, Lena Missiakas, Dominique M. Schneewind, Olaf TI Protein A Suppresses Immune Responses during Staphylococcus aureus Bloodstream Infection in Guinea Pigs SO MBIO LA English DT Article ID B-CELL SUPERANTIGEN; CONJUGATE VACCINE; ABSCESS FORMATION; SURFACE-PROTEINS; GENOME SEQUENCE; ALPHA-HEMOLYSIN; S AUREUS; COMMUNITY; RESISTANT; MODEL AB Staphylococcus aureus infection is not associated with the development of protective immunity, and disease relapses occur frequently. We hypothesize that protein A, a factor that binds immunoglobulin Fc gamma and cross-links V(H)3 clan B cell receptors (IgM), is the staphylococcal determinant for host immune suppression. To test this, vertebrate IgM was examined for protein A cross-linking. High V(H)3 binding activity occurred with human and guinea immunoglobulin, whereas mouse and rabbit immunoglobulins displayed little and no binding, respectively. Establishing a guinea pig model of S. aureus bloodstream infection, we show that protein A functions as a virulence determinant and suppresses host B cell responses. Immunization with SpA(KKAA), which cannot bind immunoglobulin, elicits neutralizing antibodies that enable guinea pigs to develop protective immunity. IMPORTANCE Staphylococcus aureus is the leading cause of soft tissue and bloodstream infections; however, a vaccine with clinical efficacy is not available. Using mice to model staphylococcal infection, earlier work identified protective antigens; however, corresponding human clinical trials did not reach their endpoints. We show that B cell receptor (IgM) cross-linking by protein A is an important immune evasion strategy of S. aureus that can be monitored in a guinea pig model of bloodstream infection. Further, immunization with nontoxigenic protein A enables infected guinea pigs to elicit antibody responses that are protective against S. aureus. Thus, the guinea pig model may support preclinical development of staphylococcal vaccines. C1 [Kim, Hwan Keun; Falugi, Fabiana; Thomer, Lena; Missiakas, Dominique M.; Schneewind, Olaf] Univ Chicago, Dept Microbiol, Chicago, IL 60637 USA. [Kim, Hwan Keun; Falugi, Fabiana; Thomer, Lena; Missiakas, Dominique M.; Schneewind, Olaf] Argonne Natl Lab, Howard Taylor Ricketts Lab, Argonne, IL 60439 USA. RP Schneewind, O (reprint author), Univ Chicago, Dept Microbiol, Chicago, IL 60637 USA. EM oschnee@bsd.uchicago.edu FU National Institute of Allergy and Infectious Diseases Infectious Diseases Branch [AI038897, AI052474] FX This work was supported by grants AI038897 and AI052474 from the National Institute of Allergy and Infectious Diseases Infectious Diseases Branch to O.S. Hwan Keun Kim, Dominique M. Missiakas, and Olaf Schneewind are inventors of patent applications related to the development of S. aureus vaccines that are currently under commercial license. NR 69 TC 0 Z9 0 U1 1 U2 7 PU AMER SOC MICROBIOLOGY PI WASHINGTON PA 1752 N ST NW, WASHINGTON, DC 20036-2904 USA SN 2150-7511 J9 MBIO JI mBio PD JAN-FEB PY 2015 VL 6 IS 1 AR e02369-14 DI 10.1128/mBio.02369-14 PG 11 WC Microbiology SC Microbiology GA CC8PZ UT WOS:000350631900037 ER PT J AU Shi, BC Chang, M Martin, J Mitreva, M Lux, R Klokkevold, P Sodergren, E Weinstock, GM Haake, SK Li, HY AF Shi, Baochen Chang, Michaela Martin, John Mitreva, Makedonka Lux, Renate Klokkevold, Perry Sodergren, Erica Weinstock, George M. Haake, Susan K. Li, Huiying TI Dynamic Changes in the Subgingival Microbiome and Their Potential for Diagnosis and Prognosis of Periodontitis SO MBIO LA English DT Article ID TREPONEMA-DENTICOLA; DISEASE; HEALTH; BACTERIA; CHEMOTAXIS; DISCOVERY; VISUALIZATION; DIVERSITY; MOTILITY AB The human microbiome influences and reflects the health or disease state of the host. Periodontitis, a disease affecting about half of American adults, is associated with alterations in the subgingival microbiome of individual tooth sites. Although it can be treated, the disease can reoccur and may progress without symptoms. Without prognostic markers, follow-up examinations are required to assess reoccurrence and disease progression and to determine the need for additional treatments. To better identify and predict the disease progression, we aim to determine whether the subgingival microbiome can serve as a diagnosis and prognosis indicator. Using metagenomic shotgun sequencing, we characterized the dynamic changes in the subgingival microbiome in periodontitis patients before and after treatment at the same tooth sites. At the taxonomic composition level, the periodontitis-associated microorganisms were significantly shifted from highly correlated in the diseased state to poorly correlated after treatment, suggesting that coordinated interactions among the pathogenic microorganisms are essential to disease pathogenesis. At the functional level, we identified disease-associated pathways that were significantly altered in relative abundance in the two states. Furthermore, using the subgingival microbiome profile, we were able to classify the samples to their clinical states with an accuracy of 81.1%. Follow-up clinical examination of the sampled sites supported the predictive power of the microbiome profile on disease progression. Our study revealed the dynamic changes in the subgingival microbiome contributing to periodontitis and suggested potential clinical applications of monitoring the subgingival microbiome as an indicator in disease diagnosis and prognosis. IMPORTANCE Periodontitis is a common oral disease. Although it can be treated, the disease may reoccur without obvious symptoms. Current clinical examination parameters are useful in disease diagnosis but cannot adequately predict the outcome of individual tooth sites after treatment. A link between the subgingival microbiota and periodontitis was identified previously; however, it remains to be investigated whether the microbiome can serve as a diagnostic and prognostic indicator. In this study, for the first time, we characterized the subgingival microbiome of individual tooth sites before and after treatment using a large-scale metagenomic analysis. Our longitudinal study revealed changes in the microbiota in taxonomic composition, cooccurrence of subgingival microorganisms, and functional composition. Using the microbiome profiles, we were able to classify the clinical states of subgingival plaque samples with a high accuracy. Follow-up clinical examination of sampled sites indicates that the subgingival microbiome profile shows promise for the development of diagnostic and prognostic tools. C1 [Shi, Baochen; Li, Huiying] Univ Calif Los Angeles, David Geffen Sch Med, Crump Inst Mol Imaging, Dept Mol & Med Pharmacol, Los Angeles, CA 90095 USA. [Chang, Michaela; Lux, Renate; Klokkevold, Perry; Haake, Susan K.] Univ Calif Los Angeles, Sch Dent, Sect Periodont, Los Angeles, CA 90024 USA. [Martin, John; Mitreva, Makedonka] Washington Univ, Genome Inst, St Louis, MO USA. [Sodergren, Erica; Weinstock, George M.] Jackson Lab Genom Med, Farmington, CT USA. [Li, Huiying] UCLA DOE Inst Genom & Prote, Los Angeles, CA USA. RP Li, HY (reprint author), Univ Calif Los Angeles, David Geffen Sch Med, Crump Inst Mol Imaging, Dept Mol & Med Pharmacol, Los Angeles, CA 90095 USA. EM huiying@mednet.ucla.edu FU NIH/NIDCR [RC1 DE020298, R01 DE021574] FX This study was supported by NIH/NIDCR grants RC1 DE020298 and R01 DE021574. NR 49 TC 6 Z9 6 U1 0 U2 12 PU AMER SOC MICROBIOLOGY PI WASHINGTON PA 1752 N ST NW, WASHINGTON, DC 20036-2904 USA SN 2150-7511 J9 MBIO JI mBio PD JAN-FEB PY 2015 VL 6 IS 1 AR e01926-14 DI 10.1128/mBio.01926-14 PG 11 WC Microbiology SC Microbiology GA CC8PZ UT WOS:000350631900061 PM 25691586 ER PT J AU Zhou, JZ He, ZL Yang, YF Deng, Y Tringe, SG Alvarez-Cohen, L AF Zhou, Jizhong He, Zhili Yang, Yunfeng Deng, Ye Tringe, Susannah G. Alvarez-Cohen, Lisa TI High-Throughput Metagenomic Technologies for Complex Microbial Community Analysis: Open and Closed Formats SO MBIO LA English DT Review ID 16S RIBOSOMAL-RNA; ANTIBIOTIC-RESISTANCE GENES; 50-MER OLIGONUCLEOTIDE ARRAYS; MICROARRAY-BASED ANALYSIS; HUMAN GUT MICROBIOTA; SEA OIL PLUME; UNCULTURED MICROORGANISMS; DEEP-SEA; HETEROLOGOUS EXPRESSION; PHYLOGENETIC MICROARRAY AB Understanding the structure, functions, activities and dynamics of microbial communities in natural environments is one of the grand challenges of 21st century science. To address this challenge, over the past decade, numerous technologies have been developed for interrogating microbial communities, of which some are amenable to exploratory work (e. g., high-throughput sequencing and phenotypic screening) and others depend on reference genes or genomes (e. g., phylogenetic and functional gene arrays). Here, we provide a critical review and synthesis of the most commonly applied "open-format" and "closed-format" detection technologies. We discuss their characteristics, advantages, and disadvantages within the context of environmental applications and focus on analysis of complex microbial systems, such as those in soils, in which diversity is high and reference genomes are few. In addition, we discuss crucial issues and considerations associated with applying complementary high-throughput molecular technologies to address important ecological questions. C1 [Zhou, Jizhong; He, Zhili; Deng, Ye] Univ Oklahoma, Inst Environm Genom, Norman, OK 73019 USA. [Zhou, Jizhong; He, Zhili; Deng, Ye] Univ Oklahoma, Dept Microbiol & Plant Biol, Norman, OK 73019 USA. [Zhou, Jizhong; Yang, Yunfeng] Tsinghua Univ, Sch Environm, State Key Joint Lab Environm Simulat & Pollut Con, Beijing 100084, Peoples R China. [Zhou, Jizhong; Alvarez-Cohen, Lisa] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Earth Sci, Berkeley, CA 94720 USA. [Deng, Ye] Chinese Acad Sci, RCEES, Beijing, Peoples R China. [Tringe, Susannah G.] Dept Energy Joint Genome Inst, Walnut Creek, CA USA. [Alvarez-Cohen, Lisa] Univ Calif Berkeley, Dept Civil & Environm Engn, Berkeley, CA 94720 USA. RP Zhou, JZ (reprint author), Univ Oklahoma, Inst Environm Genom, Norman, OK 73019 USA. EM jzhou@ou.edu OI Tringe, Susannah/0000-0001-6479-8427; ?, ?/0000-0002-7584-0632 FU U.S. Department of Energy (DOE), Office of Science, Office of Biological and Environmental Research's (OBER) Genomics Science Program to Lawrence Berkeley National Laboratory (LBNL); OBER Biological Systems Research on the Role of Microbial Communities in Carbon Cycling program [DE-SC0004601]; U.S. National Science Foundation (NSF) MacroSystems Biology program [EF-1065844]; NSF [CBET-1336709]; Strategic Environmental Research and Development Program [ER-1587]; National Institute of Environmental Health Sciences Superfund [P42ES004705]; DOE Early Career Research Program [KP/CH57/1]; DOE Office of Science [DE-AC02-05CH11231]; Collaborative Innovation Center for Regional Environmental Quality; State Key Joint Laboratory of Environment Simulation and Pollution Control at Tsinghua University FX The efforts in preparing this review were supported, through contract DE-AC02-05CH11231 (as part of ENIGMA, a Scientific Focus Area), by funding from the U.S. Department of Energy (DOE), Office of Science, Office of Biological and Environmental Research's (OBER) Genomics Science Program to Lawrence Berkeley National Laboratory (LBNL), by the OBER Biological Systems Research on the Role of Microbial Communities in Carbon Cycling program (DE-SC0004601), by the U.S. National Science Foundation (NSF) MacroSystems Biology program through grant EF-1065844 to J.Z. and Z.H. and NSF CBET-1336709 to L.A.-C., by Strategic Environmental Research and Development Program grant ER-1587 and National Institute of Environmental Health Sciences Superfund grant P42ES004705 to L.A.-C., by DOE Early Career Research Program grant no. KP/CH57/1 to S.G.T., and by the DOE Office of Science under contract no. DE-AC02-05CH11231 to DOE-Joint Genome Institute (JGI)/LBNL. This work was also supported by funding from the Collaborative Innovation Center for Regional Environmental Quality and State Key Joint Laboratory of Environment Simulation and Pollution Control at Tsinghua University to J.Z. NR 165 TC 33 Z9 34 U1 39 U2 164 PU AMER SOC MICROBIOLOGY PI WASHINGTON PA 1752 N ST NW, WASHINGTON, DC 20036-2904 USA SN 2150-7511 J9 MBIO JI mBio PD JAN-FEB PY 2015 VL 6 IS 1 AR e02288-14 DI 10.1128/mBio.02288-14 PG 17 WC Microbiology SC Microbiology GA CC8PZ UT WOS:000350631900064 ER PT J AU Xu, YT Guo, Y Li, C Zhou, XY Tucker, MC Fu, XZ Sun, R Wong, CP AF Xu, Yi-Tao Guo, Ying Li, Chang Zhou, Xuan-Yu Tucker, Michael C. Fu, Xian-Zhu Sun, Rong Wong, Ching-Ping TI Graphene oxide nano-sheets wrapped Cu2O microspheres as improved performance anode materials for lithium ion batteries SO NANO ENERGY LA English DT Article DE Graphene oxide nano-sheets; Cu2O microspheres; Lithium ion batteries; 3D; Anode materials; In-situ electrochemical reduction ID ELECTROCHEMICAL PERFORMANCE; ELECTRODE MATERIALS; PHOTOCATALYTIC ACTIVITY; ENERGY-STORAGE; GRAPHITE OXIDE; POROUS CARBON; COMPOSITE; NANOCRYSTALS; FABRICATION; PAPER AB Cu2O microspheres were successfully encapsulated by graphene oxide (GO) nano-sheets and used directly as the anode material for lithium ion batteries. The core-shell structured Cu2O@GO composite delivered a reversible capacity of 458 mA h g(-1) at a current density of 100 mA g(-1) after 50 cycles. Even at a high charge-discharge rate of 1000 mA g(-1), Cu2O@GO still demonstrated a reversible capacity of 240 mA h g(-1) after 200 cycles, significantly higher than those of the bare Cu2O microspheres (37 mA h g(-1)) and GO nano-sheets (11 mA h g(-1)). The rate capability evaluated by the ratio of capacity at 100 mA g(-1)/1000 mA g(-1) current density was 49%, 25% and 9.8% for Cu2O@GO, bare Cu2O and GO, respectively. The greatly enhanced performance for GO nano-sheets wrapped Cu2O microspheres composite mainly resulted from the synergistic effect of Cu2O microspheres and GO nano-sheets core-shell composite: the flexible in-situ electrochemically reduced GO nano-sheet coating layer functioning as an efficient three dimensional (3D) conductive network and lithium storage active material; the Cu2O microsphere core functioning as a skeleton to support multilayer GO sheets and avoid GO nano-sheets aggregation. (C) 2014 Elsevier Ltd. All rights reserved. C1 [Xu, Yi-Tao; Guo, Ying; Li, Chang; Zhou, Xuan-Yu; Fu, Xian-Zhu; Sun, Rong; Wong, Ching-Ping] Chinese Acad Sci, Shenzhen Inst Adv Technol, Shenzhen 518055, Peoples R China. [Xu, Yi-Tao] Univ Sci & Technol China, Inst Nano Sci & Technol, Suzhou 215123, Peoples R China. [Tucker, Michael C.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. [Wong, Ching-Ping] Chinese Univ Hong Kong, Dept Elect Engn, Hong Kong, Hong Kong, Peoples R China. [Wong, Ching-Ping] Georgia Inst Technol, Sch Mat Sci & Engn, Atlanta, GA 30332 USA. RP Fu, XZ (reprint author), Chinese Acad Sci, Shenzhen Inst Adv Technol, Shenzhen 518055, Peoples R China. EM xz.fu@siat.ac.cn; rong.sun@siat.ac.cn FU National Natural Science Foundation of China [21203236]; Guangdong and Shenzhen Innovative Research Team Program [2011D052, KYPT20121228160843692]; Shenzhen basic research plan [JC201005270372A] FX This work was financially supported by the National Natural Science Foundation of China (no. 21203236), Guangdong and Shenzhen Innovative Research Team Program (nos. 2011D052, KYPT20121228160843692), and Shenzhen basic research plan (JC201005270372A). NR 39 TC 31 Z9 33 U1 49 U2 217 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 2211-2855 EI 2211-3282 J9 NANO ENERGY JI Nano Energy PD JAN PY 2015 VL 11 BP 38 EP 47 DI 10.1016/j.nanoen.2014.10.011 PG 10 WC Chemistry, Physical; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA CD6JB UT WOS:000351194300005 ER PT J AU Tian, M Wang, W Liu, Y Jungjohann, KL Harris, CT Lee, YC Yang, RG AF Tian, Miao Wang, Wei Liu, Yang Jungjohann, Katherine L. Harris, C. Thomas Lee, Yung-Cheng Yang, Ronggui TI A three-dimensional carbon nano-network for high performance lithium ion batteries SO NANO ENERGY LA English DT Article DE Three-dimensional nano-network; Carbon; Li-ion battery; Anode ID ATOMIC LAYER DEPOSITION; HYBRID ELECTRIC VEHICLES; REDUCED GRAPHENE OXIDE; ENERGY-STORAGE; ELECTROCHEMICAL PERFORMANCE; MICROBATTERY APPLICATIONS; ANODE MATERIAL; TIO2 ANATASE; NANOTUBES; COMPOSITE AB Three-dimensional (3D) network structure has been envisioned as a superior architecture for lithium ion battery (LIB) electrodes, which enhances both ion and electron transport to significantly improve battery performance. Herein, a 3D carbon nano-network is fabricated through chemical vapor deposition of carbon on a scalably manufactured 3D porous anodic alumina (PAA) template. As a demonstration on the applicability of 3D carbon nano-network for LIB electrodes, the low conductivity active material, TiO2, is then uniformly coated on the 3D carbon nano-network using atomic layer deposition. High power performance is demonstrated in the 3D C/TiO2 electrodes, where the parallel tubes and gaps in the 3D carbon nano-network facilitates fast Li ion transport. A large areal capacity of similar to 0.37 mAh cm(-2) is achieved due to the large TiO2 mass loading in the 60 pm-thick 3D C/TiO2 electrodes. At a test rate of C/5, the 3D C/TiO2 electrode with 18 nm-thick TiO2 delivers a high gravimetric capacity of similar to 240 mAh g(-1), calculated with the mass of the whole electrode. A long cycle life of over 1000 cycles with a capacity retention of 91% is demonstrated at 1C. The effects of the electrical conductivity of carbon nano-network, ion diffusion, and the electrolyte permeability on the rate performance of these 3D C/TiO2 electrodes are systematically studied. (C) 2014 Elsevier Ltd. All rights reserved. C1 [Tian, Miao; Lee, Yung-Cheng; Yang, Ronggui] Univ Colorado, Dept Mech Engn, Boulder, CO 80309 USA. [Wang, Wei] Chinese Acad Sci, Ningbo Inst Mat Technol & Engn, Adv Liion Batteries Engn Lab, Ningbo 315201, Zhejiang, Peoples R China. [Liu, Yang; Jungjohann, Katherine L.; Harris, C. Thomas] Sandia Natl Labs, Ctr Integrated Nanotechnol CINT, Albuquerque, NM 87123 USA. RP Yang, RG (reprint author), Univ Colorado, Dept Mech Engn, Boulder, CO 80309 USA. EM ronggui.yang@colorado.edu RI Yang, Ronggui/H-1278-2011; Wang, Wei/B-3556-2012 FU DARPA Center on Nanoscale Science and Technology for Integrated Micro/Nano-Electro-mechanical Transducers (iMINT) - Defense Advanced Research Projects Agency (DARPA) N/MEMS S&T Fundamentals program [N66001-10-1-4007]; NNIN; National Science Foundation [ECS-0335765]; U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX This work was supported by the DARPA Center on Nanoscale Science and Technology for Integrated Micro/Nano-Electro-mechanical Transducers (iMINT), supported by the Defense Advanced Research Projects Agency (DARPA) N/MEMS S&T Fundamentals program under grant no. N66001-10-1-4007 issued by the Space and Naval Warfare Systems Center Pacific (SPAWAR). Some of the micro/nano-fabrication work was conducted in the Colorado Nanofabrication Laboratories, supported in part by the NNIN and the National Science Foundation under Grant No. ECS-0335765. The TEM characterization work was performed at the Center for Integrated Nanotechnologies, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science. Sandia National Laboratories is a multiprogram laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000. NR 70 TC 14 Z9 14 U1 17 U2 134 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 2211-2855 EI 2211-3282 J9 NANO ENERGY JI Nano Energy PD JAN PY 2015 VL 11 BP 500 EP 509 DI 10.1016/j.nanoen.2014.11.006 PG 10 WC Chemistry, Physical; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA CD6JB UT WOS:000351194300051 ER PT J AU Xing, ZY Wang, B Gao, WY Pan, CQ Halsted, JK Chong, ES Lu, J Wang, XF Luo, W Chang, CH Wen, YH Ma, SQ Amine, K Ji, XL AF Xing, Zhenyu Wang, Bao Gao, Wenyang Pan, Changqing Halsted, Joshua K. Chong, Elliot S. Lu, Jun Wang, Xingfeng Luo, Wei Chang, Chih-Hung Wen, Youhai Ma, Shengqian Amine, Khalil Ji, Xiulei TI Reducing CO2 to dense nanoporous graphene by Mg/Zn for high power electrochemical capacitors SO NANO ENERGY LA English DT Article DE CO2 reduction; Nanoporous graphene; Magnesiothermic reduction; Electrochemical capacitors ID ULTRAHIGH-ENERGY DENSITY; HIGH-PERFORMANCE; GRAPHITE OXIDE; MICRO-SUPERCAPACITORS; CHEMICAL-REDUCTION; CARBON-DIOXIDE; STORAGE; FILMS; ULTRACAPACITORS; ELECTRODES AB Converting CO2 to valuable materials is attractive. Herein, we report using simple metallothermic reactions to reduce atmospheric CO2 to dense nanoporous graphene. By using a Zn/Mg mixture as a reductant, the resulted nanoporous graphene exhibits highly desirable properties: high specific surface area of 1900 m(2)/g, a great conductivity of 1050 S/m and a tap density of 0.63 g/cm(3), comparable to activated carbon. The nanoporous graphene contains a fine mesoporous structure constructed by curved few-layer graphene nanosheets. The unique property ensemble enables one of the best high-rate performances reported for electrochemical capacitors: a specific capacitance of similar to 170 F/g obtained at 2000 mV/s and 40 F/g at a frequency of 120 Hz. This simple fabricating strategy conceptually provides opportunities for materials scientists to design and prepare novel carbon materials with metallothermic reactions. (C) 2014 Elsevier Ltd. All rights reserved. C1 [Xing, Zhenyu; Wang, Bao; Halsted, Joshua K.; Chong, Elliot S.; Wang, Xingfeng; Luo, Wei; Ji, Xiulei] Oregon State Univ, Dept Chem, Corvallis, OR 97331 USA. [Lu, Jun; Amine, Khalil] Argonne Natl Lab, Lemont, IL 60439 USA. [Pan, Changqing; Chang, Chih-Hung] Oregon State Univ, Sch Chem Biol & Environm Engn, Corvallis, OR 97331 USA. [Wen, Youhai] Natl Energy Technol Lab, Albany, OR 97321 USA. [Gao, Wenyang; Ma, Shengqian] Univ S Florida, Dept Chem, Tampa, FL 33620 USA. RP Amine, K (reprint author), Argonne Natl Lab, Lemont, IL 60439 USA. EM amine@anl.gov; david.ji@oregonstate.edu RI Wang, Bao/G-9032-2015; Luo, Wei/E-1582-2011; Ma, Shengqian/B-4022-2012; Halsted, Joshua/P-4605-2014 OI Luo, Wei/0000-0002-4019-4634; Ma, Shengqian/0000-0002-1897-7069; Halsted, Joshua/0000-0001-6986-3072 FU Oregon State University FX X. J. gratefully acknowledges the financial support from Oregon State University. We would like to thank Dr. Peter Eschbach and Ms. Teresa Sawyer for the SEM measurements at the OSU Electron Microscopy Facility. Additional acknowledgments extend out to Mr. Joshua Razink for the TEM measurements at the Center for Advanced Materials Characterization at Oregon (CAMCOR) at the University of Oregon. NR 60 TC 19 Z9 19 U1 17 U2 78 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 2211-2855 EI 2211-3282 J9 NANO ENERGY JI Nano Energy PD JAN PY 2015 VL 11 BP 600 EP 610 DI 10.1016/j.nanoen.2014.11.011 PG 11 WC Chemistry, Physical; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA CD6JB UT WOS:000351194300062 ER PT J AU Papadas, IT Subrahmanyam, KS Kanatzidis, MG Armatas, GS AF Papadas, I. T. Subrahmanyam, K. S. Kanatzidis, M. G. Armatas, G. S. TI Templated assembly of BiFeO3 nanocrystals into 3D mesoporous networks for catalytic applications SO NANOSCALE LA English DT Article ID LIGHT PHOTOCATALYTIC PROPERTIES; THIN-FILM HETEROSTRUCTURES; VISIBLE-LIGHT; BISMUTH FERRITE; METAL NANOPARTICLES; P-NITROPHENOL; REDUCTION; ADSORPTION; FIELDS AB The self-assembly of uniform nanocrystals into large porous architectures is currently of immense interest for nanochemistry and nanotechnology. These materials combine the respective advantages of discrete nanoparticles and mesoporous structures. In this article, we demonstrate a facile nanoparticle templating process to synthesize a three-dimensional mesoporous BiFeO3 material. This approach involves the polymer-assisted aggregating assembly of 3-aminopropanoic acid-stabilized bismuth ferrite (BiFeO3) nanocrystals followed by thermal decomposition of the surfactant. The resulting material consists of a network of tightly connected BiFeO3 nanoparticles (similar to 6-7 nm in diameter) and has a moderately high surface area (62 m(2) g(-1)) and uniform pores (ca. 6.3 nm). As a result of the unique mesostructure, the porous assemblies of BiFeO3 nanoparticles show an excellent catalytic activity and chemical stability for the reduction of p-nitrophenol to p-aminophenol with NaBH4. C1 [Papadas, I. T.; Armatas, G. S.] Univ Crete, Dept Mat Sci & Technol, Iraklion 71003, Crete, Greece. [Subrahmanyam, K. S.; Kanatzidis, M. G.] Northwestern Univ, Dept Chem, Evanston, IL 60208 USA. [Kanatzidis, M. G.] Argonne Natl Lab, Div Mat Sci, Argonne, IL 60439 USA. RP Armatas, GS (reprint author), Univ Crete, Dept Mat Sci & Technol, Iraklion 71003, Crete, Greece. EM garmatas@materials.uoc.gr RI Armatas, Gerasimos/F-4753-2011; OI Armatas, Gerasimos/0000-0001-9475-1929; Papadas, Ioannis/0000-0003-4718-1411 FU Greek Ministry of Education (NSRF); European Union under the ERC Grant Schemes (MESOPOROUS-NPs) [ERC-09]; European Union under THALES [MIS 80802]; NEUP grant from the Department of Energy, Office of Nuclear Energy FX We acknowledge support from the Greek Ministry of Education (NSRF) and the European Union under the ERC Grant Schemes (ERC-09, MESOPOROUS-NPs) and THALES project (MIS 80802). Research at Northwestern University was supported by a NEUP grant from the Department of Energy, Office of Nuclear Energy. NR 42 TC 7 Z9 7 U1 14 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 2015 VL 7 IS 13 BP 5737 EP 5743 DI 10.1039/c5nr00185d PG 7 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA CE2CD UT WOS:000351619600023 PM 25743612 ER PT J AU Mueller, DN Machala, ML Bluhm, H Chueh, WC AF Mueller, David N. Machala, Michael L. Bluhm, Hendrik Chueh, William C. TI Redox activity of surface oxygen anions in oxygen-deficient perovskite oxides during electrochemical reactions SO NATURE COMMUNICATIONS LA English DT Article ID RAY-ABSORPTION-SPECTROSCOPY; ELECTRONIC-STRUCTURE; TRANSITION-METAL; FUEL-CELLS; CHARGE COMPENSATION; MODEL; ION; NONSTOICHIOMETRY; LA1-XSRXFEO3; SEGREGATION AB Surface redox-active centres in transition-metal oxides play a key role in determining the efficacy of electrocatalysts. The extreme sensitivity of surface redox states to temperatures, to gas pressures and to electrochemical reaction conditions renders them difficult to investigate by conventional surface-science techniques. Here we report the direct observation of surface redox processes by surface-sensitive, operando X-ray absorption spectroscopy using thin-film iron and cobalt perovskite oxides as model electrodes for elevated-temperature oxygen incorporation and evolution reactions. In contrast to the conventional view that the transition metal cations are the dominant redox-active centres, we find that the oxygen anions near the surface are a significant redox partner to molecular oxygen due to the strong hybridization between oxygen 2p and transition metal 3d electronic states. We propose that a narrow electronic state of significant oxygen 2p character near the Fermi level exchanges electrons with the oxygen adsorbates. This result highlights the importance of surface anion-redox chemistry in oxygen-deficient transition-metal oxides. C1 [Mueller, David N.; Machala, Michael L.; Chueh, William C.] Stanford Univ, Dept Mat Sci & Engn, Stanford, CA 94305 USA. [Bluhm, Hendrik] Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA. [Chueh, William C.] Stanford Inst Mat & Energy Sci, SLAC Natl Accelerator Lab, Menlo Pk, CA 94025 USA. RP Chueh, WC (reprint author), Stanford Univ, Dept Mat Sci & Engn, 496 Lomita Mall, Stanford, CA 94305 USA. EM wchueh@stanford.edu RI Mueller, David/Q-6371-2016 OI Mueller, David/0000-0002-1062-6985 FU US Department of Energy, Office of Fossil Energy [DE-FE0009620]; Department of Energy, Laboratory Directed Research and Development funding [DE-AC02-76SF00515]; Division of Chemical Sciences, Geosciences, and Biosciences of the US Department of Energy at the Lawrence Berkeley National Laboratory [DE-AC02-05CH11231]; National Science Foundation [DGE-114747] FX The materials component of this work was supported by the US Department of Energy, Office of Fossil Energy, Grant No. DE-FE0009620; and the X-ray spectroscopy component was supported by the Department of Energy, Laboratory Directed Research and Development funding, under contract DE-AC02-76SF00515. The ALS and the Molecular Environmental Sciences beamline 11.0.2 are supported by the Director, Office of Science, Office of Basic Energy Sciences, and the Division of Chemical Sciences, Geosciences, and Biosciences of the US Department of Energy at the Lawrence Berkeley National Laboratory under Contract No. DE-AC02-05CH11231. M.L.M. was supported by the National Science Foundation Graduate Research Fellowship under Grant No. DGE-114747. We thank A.H. McDaniel, F. El Gabaly (Sandia National Laboratories), M. Ng, A. Shavorskiy, O. Karslioglu, I. Zegkinoglou (Lawrence Berkeley National Laboratory), I. Leung, A. Feng, Y. Shi and X. Ye (Stanford University) for experimental assistance. We also thank T. Devereaux, B. Moritz, C. Li, C. Jia (Stanford University/SLAC National Accelerator Laboratory) and F. M. F. de Groot (Utrecht University) for insightful discussions. NR 52 TC 40 Z9 40 U1 27 U2 172 PU NATURE PUBLISHING GROUP PI LONDON PA MACMILLAN BUILDING, 4 CRINAN ST, LONDON N1 9XW, ENGLAND SN 2041-1723 J9 NAT COMMUN JI Nat. Commun. PD JAN PY 2015 VL 6 AR 6097 DI 10.1038/ncomms7097 PG 8 WC Multidisciplinary Sciences SC Science & Technology - Other Topics GA CE5FU UT WOS:000351857300001 PM 25598003 ER PT J AU Amaral, SV Bevelhimer, MS Cada, GF Giza, DJ Jacobson, PT McMahon, BJ Pracheil, BM AF Amaral, Stephen V. Bevelhimer, Mark S. Cada, Glenn F. Giza, Daniel J. Jacobson, Paul T. McMahon, Brian J. Pracheil, Brenda M. TI Evaluation of Behavior and Survival of Fish Exposed to an Axial-Flow Hydrokinetic Turbine SO NORTH AMERICAN JOURNAL OF FISHERIES MANAGEMENT LA English DT Article ID ATLANTIC SALMON; AMERICAN SHAD; SMOLTS; WATER; MARK AB Previous studies have evaluated fish injury and mortality at hydrokinetic (HK) turbines, but because these studies focused on the impacts of these turbines in situ they were unable to evaluate fish responses to controlled environmental characteristics (e.g., current velocity and light or dark conditions). In this study, we used juvenile hybrid Striped Bass (HSB; Striped Bass Morone saxatilis x White Bass M. chrysops; N = 620), Rainbow Trout Oncorhynchus mykiss (N = 3,719), and White Sturgeon Acipenser transmontanus (N = 294) in a series of laboratory experiments to (1) evaluate the ability of fish to avoid entrainment through an axial-flow HK turbine, (2) evaluate fish injury and survival associated with turbine entrainment, and (3) compare the effects of different HK turbines on fish. We found that the probability of turbine entrainment was species dependent and highest for HSB. Across species, current velocity influenced entrainment probability. Among entrained fish, observed survival rates were generally >0.95. The probability of injury for surviving entrained fish only differed from that for nonentrained fish for Rainbow Trout and in general was not >0.20. The probability of injury following entrainment was greater only for HSB, although there were no differences in injury rates between fish that were turbine entrained and those that were not, suggesting that injuries were not turbine related. Taking turbine entrainment, survival, and injury estimates together allowed us to estimate the probability of a randomly selected fish in a population proximate to an HK turbine surviving passage or remaining uninjured after passage. For species and current velocities for which there was a significant effect due to entrainment, we estimated, for instance, that HSB had a survival probability of 0.95 and that Rainbow Trout and White Sturgeon had a >0.99 probability of survival. Similarly, by combining these estimates with those from previous studies, we derived total passage survival probabilities >0.90 but generally approaching 1.00 across different HK turbine types, fish species, and fish lengths. C1 [Amaral, Stephen V.; Giza, Daniel J.; McMahon, Brian J.] Alden Res Lab Inc, Holden, MA 01520 USA. [Bevelhimer, Mark S.; Cada, Glenn F.; Pracheil, Brenda M.] Oak Ridge Natl Lab, Div Environm Sci, Oak Ridge, TN 37831 USA. [Jacobson, Paul T.] Elect Power Res Inst, Columbia, MD 21044 USA. RP Pracheil, BM (reprint author), Oak Ridge Natl Lab, Div Environm Sci, 1 Bethel Valley Rd, Oak Ridge, TN 37831 USA. EM pracheilbm@ornl.gov FU U.S. Department of Energy and Electric Power Research Institute; U.S. Department of Energy's (DOE) Energy Efficiency and Renewable Energy Office, Wind and Water Power Technologies Program through Oak Ridge National Laboratory [DE-AC05-00OR22725] FX We thank E. Lovelace (formerly with Free Flow Power) and T. Pham (Massachusetts Maritime Academy) for technical turbine assistance, Alabama Power for use of their DIDSON unit, and N. Lucia, J. Muise, and S. St. Jean of Alden Laboratories for laboratory technical assistance. We also thank J. Brown-Saracino, S. Bickel, and three anonymous reviewers for manuscript comments. This study was funded by the U.S. Department of Energy and Electric Power Research Institute. G.F.C., M.S.B., and B.M.P. were supported by the U.S. Department of Energy's (DOE) Energy Efficiency and Renewable Energy Office, Wind and Water Power Technologies Program through Oak Ridge National Laboratory, which is managed by UT-Battelle, LLC, for the DOE under contract DE-AC05-00OR22725. Opinions expressed are those of the authors and do not reflect those of their employers. NR 34 TC 3 Z9 3 U1 5 U2 16 PU TAYLOR & FRANCIS INC PI PHILADELPHIA PA 530 WALNUT STREET, STE 850, PHILADELPHIA, PA 19106 USA SN 0275-5947 EI 1548-8675 J9 N AM J FISH MANAGE JI North Am. J. Fish Manage. PY 2015 VL 35 IS 1 BP 97 EP 113 DI 10.1080/02755947.2014.982333 PG 17 WC Fisheries SC Fisheries GA CD9VN UT WOS:000351447600009 ER PT J AU Koschny, R Krupp, W Xu, LX Mueller, WC Bauer, M Sinn, P Keller, M Koschny, T Walczak, H Bruckner, T Ganten, TM Holland, H AF Koschny, Ronald Krupp, Wolfgang Xu, Li-Xin Mueller, Wolf C. Bauer, Manfred Sinn, Peter Keller, Marius Koschny, Thomas Walczak, Henning Bruckner, Thomas Ganten, Tom M. Holland, Heidrun TI WHO grade related expression of TRAIL-receptors and apoptosis regulators in meningioma SO PATHOLOGY RESEARCH AND PRACTICE LA English DT Article DE Meningioma; Immunohistochemistry; TRAIL-receptor; Apoptosis regulators ID HEPATOCELLULAR-CARCINOMA; ANTICANCER THERAPY; DEATH RECEPTORS; LIGAND TRAIL; CANCER-CELLS; RESISTANCE; CASPASE-8; SURVIVAL; CFLIP; BCL-2 AB Background and aims: The expression of the tumor necrosis factor-related apoptosis-inducing ligand (TRAIL) receptors and key regulators of the extrinsic apoptosis pathway correlate with clinical features and the WHO grade of malignancy in some tumor entities. Expression of pro-apoptotic TRAIL receptors and executioners of apoptosis are a prerequisite for TRAIL-based therapies as a promising future targeted therapy. Methods: Human meningioma tissues (n = 24 WHO grade I, n = 7 WHO grade II, n = 6 WHO grade III) were immunohistochemically analyzed for the expression of TRAIL-R1, TRAIL-R2, TRAIL-R3, TRAIL-R4, caspase-8, cFLIP, Bc1-2, Bcl-XL, Mcl-1, Bax, and Bak. Staining intensities were quantified by an automated software-based algorithm. Results: While TRAIL-R1 and TRAIL-R3 were nearly absent in meningiomas, TRAIL-R2 and TRAIL-R4 were abundantly expressed. However, only TRAIL-R4 expression correlated with the WHO grade of malignancy. Bc1-2 showed a non-significant upregulation in WHO grade III meningiomas. Bcl-XL and Mc1-1 expression was significantly higher in WHO grade II compared to grade I. Bcl-XL and TRAIL-R4 expression correlated with the mitotic activity (Ki67) of the tumor. Furthermore, TRAIL-R2 expression correlated with TRAIL-R4. Bak expression correlated with both, Bcl-XL and Mc1-1 expression. The expression patterns did neither correlate with the progression-free nor with the overall survival of the meningioma patients. Conclusions: Apoptosis-inducing TRAIL-R2 and all key executioners of the extrinsic apoptosis pathway are abundantly expressed in meningioma. For some regulators of apoptosis with opposite functions, the expression of the pro-apoptotic protein significantly correlated with the expression level of the respective anti-apoptotic binding partner, possibly resulting in a steady-state of apoptosis. TRAIL-R2 might serve as a novel therapeutic target in meningioma. (C) 2014 Elsevier GmbH. All rights reserved. C1 [Koschny, Ronald; Ganten, Tom M.] Univ Heidelberg Hosp, Dept Gastroenterol, Heidelberg, Germany. [Krupp, Wolfgang; Xu, Li-Xin] Univ Leipzig, Dept Neurosurg, D-04109 Leipzig, Germany. [Xu, Li-Xin; Holland, Heidrun] Translat Ctr Regenerat Med TRM, Leipzig, Germany. [Xu, Li-Xin; Holland, Heidrun] Univ Leipzig, Fac Med, D-04109 Leipzig, Germany. [Mueller, Wolf C.; Bauer, Manfred] Univ Leipzig, Dept Neuropathol, D-04109 Leipzig, Germany. [Sinn, Peter] Univ Heidelberg Hosp, Dept Pathol, Heidelberg, Germany. [Keller, Marius] Univ Heidelberg Hosp, Dept Cardiol, Heidelberg, Germany. [Koschny, Thomas] US DOE, Ames Lab, Ames, IA 50011 USA. [Koschny, Thomas] Iowa State Univ, Dept Phys & Astron, Ames, IA USA. [Walczak, Henning] UCL Canc Inst, Ctr Cell Death Canc & Inflammat CCCI, London, England. [Bruckner, Thomas] Heidelberg Univ, Inst Med Biometry & Informat, Heidelberg, Germany. RP Koschny, R (reprint author), Dept Internal Med, Neuenheimer Feld 410, D-69120 Heidelberg, Germany. EM ronald.koschny@med.uni-heidelberg.de NR 33 TC 2 Z9 2 U1 0 U2 1 PU ELSEVIER GMBH, URBAN & FISCHER VERLAG PI JENA PA OFFICE JENA, P O BOX 100537, 07705 JENA, GERMANY SN 0344-0338 J9 PATHOL RES PRACT JI Pathol. Res. Pract. PY 2015 VL 211 IS 2 BP 109 EP 116 DI 10.1016/j.prp.2014.11.002 PG 8 WC Pathology SC Pathology GA CD5GU UT WOS:000351116800002 PM 25481563 ER PT J AU Chang, WB Russ, B Ho, V Urban, JJ Segalman, RA AF Chang, W. B. Russ, B. Ho, V. Urban, J. J. Segalman, R. A. TI Gold nanocrystal arrays as a macroscopic platform for molecular junction thermoelectrics SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID VAPOR-SENSING PROPERTIES; CHARGE-TRANSPORT; METAL NANOPARTICLES; CONTACT RESISTANCE; THERMAL TRANSPORT; LENGTH DEPENDENCE; SURFACE-CHEMISTRY; CONDUCTIVITY; CONDUCTANCE; FILMS AB Efficiencies of bulk thermoelectric systems have been limited because the Seebeck coefficient and electrical conductivity are typically inversely correlated in traditional materials. Decoupling of these properties has been demonstrated in molecular junctions by capitalizing on the unique electronic transport at organic-inorganic interfaces. In this work, the thermoelectric properties of gold nanocrystal arrays with varying thiol-terminated ligands are compared to molecular junction experiments. The experimental results and supporting theory demonstrate that gold nanocrystal arrays are a valuable model system for mapping the applicability of molecular junction design rules to the design of macroscale organic-inorganic hybrid thermoelectric materials. C1 [Chang, W. B.; Segalman, R. A.] Univ Calif Santa Barbara, Dept Mat, Santa Barbara, CA 93117 USA. [Russ, B.; Urban, J. J.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Ho, V.] Univ Calif Berkeley, Dept Biomol & Chem Engn, Berkeley, CA 94720 USA. RP Segalman, RA (reprint author), Univ Calif Santa Barbara, Dept Mat, Santa Barbara, CA 93117 USA. EM segalman@engineering.ucsb.edu RI Foundry, Molecular/G-9968-2014 FU AFOSR MURI [FA9550-12-1-0002]; Molecular Foundry, Office of Science, Office of Basic Energy Sciences, at the U.S. Department of Energy (DOE) [DE-AC02-05CH11231]; Department of Defense, AFOSR under the National Defense Science and Engineering Graduate Fellowship (DOD-NDSEG) [FA9550-11-C-0028, 32 CFR 168a] FX This work was supported by AFOSR MURI FA9550-12-1-0002. J.U. acknowledges support from the Molecular Foundry, Office of Science, Office of Basic Energy Sciences, at the U.S. Department of Energy (DOE), Contract No. DE-AC02-05CH11231. B.R. gratefully acknowledges the Department of Defense, AFOSR, for fellowship support under the National Defense Science and Engineering Graduate Fellowship (DOD-NDSEG), 32 CFR 168a under contract FA9550-11-C-0028. NR 28 TC 3 Z9 3 U1 1 U2 15 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2015 VL 17 IS 9 BP 6207 EP 6211 DI 10.1039/c4cp04465g PG 5 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA CD9RH UT WOS:000351435300004 PM 25652423 ER PT J AU Lei, Y Liu, B Lu, JL Lin, X Gao, L Guisinger, NP Greeley, JP Elam, JW AF Lei, Yu Liu, Bin Lu, Junling Lin, Xiao Gao, Li Guisinger, Nathan P. Greeley, Jeffrey P. Elam, Jeffrey W. TI Synthesis of palladium nanoparticles on TiO2(110) using a beta-diketonate precursor SO PHYSICAL CHEMISTRY CHEMICAL PHYSICS LA English DT Article ID ATOMIC LAYER DEPOSITION; REFLECTION-ABSORPTION SPECTROSCOPY; TEMPERATURE-PROGRAMMED DESORPTION; SCANNING-TUNNELING-MICROSCOPY; AUGMENTED-WAVE METHOD; SURFACE-CHEMISTRY; MO(110) SURFACE; PD ATOMS; ADSORPTION; NUCLEATION AB The adsorption of palladium hexafluoracetylacetone (Pd(hfac)(2)) and nucleation of Pd nanoparticles on TiO2(110) surface were observed using scanning tunneling microscopy (STM). Surface species of Pd(hfac)* and Ti(hfac)* uniformly adsorbed on TiO2(110) upon exposure of Pd(hfac)(2). No preferential nucleation was observed for the surface species. Atomic resolution STM images revealed that both Pd(hfac)* and Ti(hfac)* appeared on the metastable Ti(5c) sites. After annealing at 700 K, sub-nm Pd nanoparticles were observed across the TiO2(110) without preferential nucleation. The adsorption preferences of Pd(hfac), hfac, and atomic Pd on TiO2(110) surface were studied using density functional theory (DFT), and possible decomposition pathways of Pd(hfac) 2 leading to the formation of Pd nucleation sites were presented. C1 [Lei, Yu; Elam, Jeffrey W.] Argonne Natl Lab, Div Energy Syst, Lemont, IL 60439 USA. [Lei, Yu] Univ Alabama, Dept Chem & Mat Engn, Huntsville, AL 35899 USA. [Liu, Bin] Kansas State Univ, Dept Chem Engn, Manhattan, KS 66506 USA. [Lu, Junling] Univ Sci & Technol China, Dept Chem Phys, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Peoples R China. [Lu, Junling] Univ Sci & Technol China, CAS Key Lab Mat Energy Convers, Hefei 230026, Peoples R China. [Lin, Xiao] Chinese Acad Sci, Univ Chinese Acad Sci, Beijing 100049, Peoples R China. [Lin, Xiao] Chinese Acad Sci, Inst Phys, Beijing 100049, Peoples R China. [Gao, Li] Calif State Univ Northridge, Dept Phys & Astron, Northridge, CA 91330 USA. [Guisinger, Nathan P.] Argonne Natl Lab, Ctr Nanoscale Mat, Lemont, IL 60439 USA. [Greeley, Jeffrey P.] Purdue Univ, Sch Chem Engn, W Lafayette, IN 47907 USA. RP Lei, Y (reprint author), Argonne Natl Lab, Div Energy Syst, Lemont, IL 60439 USA. EM yu.lei@uah.edu; jelam@anl.gov RI Lin, Xiao/B-5055-2009; Lu, Junling/F-3791-2010; Liu, Bin/C-1475-2012; OI Lu, Junling/0000-0002-7371-8414; Lei, Yu/0000-0002-4161-5568 FU Institute for Atom-efficient Chemical Transformations (IACT), an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]; EMSL, a national scientific user facility located at Pacific Northwest National Laboratory; NERSC, the user facility located at Lawrence Berkeley National Laboratory; Argonne Laboratory Computing Resource Center (LCRC) FX This material is based upon work supported as part of the Institute for Atom-efficient Chemical Transformations (IACT), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences. 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 and user proposal CNM 24735. The authors acknowledge grants of computer time from EMSL, a national scientific user facility located at Pacific Northwest National Laboratory, NERSC, the user facility located at Lawrence Berkeley National Laboratory and the Argonne Laboratory Computing Resource Center (LCRC). We thank Zhu Liang at University of Illinois at Chicago and Bing Yang at Argonne National Laboratory for the discussions. NR 53 TC 2 Z9 2 U1 1 U2 31 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9076 EI 1463-9084 J9 PHYS CHEM CHEM PHYS JI Phys. Chem. Chem. Phys. PY 2015 VL 17 IS 9 BP 6470 EP 6477 DI 10.1039/c4cp05761a PG 8 WC Chemistry, Physical; Physics, Atomic, Molecular & Chemical SC Chemistry; Physics GA CD9RH UT WOS:000351435300035 PM 25657070 ER PT J AU Saha, D Moken, T Chen, JH Hensley, DK Delaney, K Hunt, MA Nelson, K Spurri, A Benham, L Brice, R Azoro, M AF Saha, Dipendu Moken, Tara Chen, Jihua Hensley, Dale K. Delaney, Kristen Hunt, Marcus A. Nelson, Karl Spurri, Amada Benham, Lauren Brice, Robin Azoro, Martina TI Micro-/mesoporous carbons for controlled release of antipyrine and indomethacin SO RSC ADVANCES LA English DT Article ID MESOPOROUS SILICA NANOPARTICLES; CONTROLLED DRUG-DELIVERY; WATER-SOLUBLE DRUG; IN-VITRO; SYSTEM; CHITOSAN; PH; MICROPARTICLES; PARTICLES; CARRIER AB We have demonstrated the potential of meso-and microporous carbons in controlled release applications and targeted oral drug delivery. We have employed two mesoporous and two microporous carbons for the sustained release of one water-soluble drug (antipyrine) and one water-insoluble drug (indomethacin), using these as models to examine the controlled release characteristics. The micro-/mesoporous carbons were characterized as having a BET surface area of 372-2251 m(2) g(-1) and pore volume 0.63-1.03 cm(3) g(-1). The toxicity studies with E. coli bacterial cells did not reveal significant toxicity, which is in accordance with our previous studies on human cells with similar materials. Mucin adsorption tests with type III pork mucin demonstrated 20-30% mucin adsorption by the carbon samples and higher mucin adsorption could be attributed to higher surface area and more oxygen functionalities. Antipyrine and indomethacin loading was 6-78% in these micro-/mesoporous carbons. The signatures in thermogravimetric studies revealed the presence of drug molecules within the porous moieties of the carbon. The partial shifting of the decomposition peak of the drug adsorbed within the carbon pores was caused by the confinement of drug molecules within the narrow pore space of the carbon. The release profiles of both drugs were examined in simulated gastric fluid (pH = 1.2) and in three other release media with respective pH values of 4.5, 6.8 and 7.4, along with varying residence times to simulate the physiological conditions of the stomach, duodenum, small intestine and colon, respectively. All the release profiles manifested diffusion controlled sustained release that corroborates the effective role of micro-/mesoporous carbons as potential drug carriers. C1 [Saha, Dipendu; Moken, Tara; Nelson, Karl; Spurri, Amada; Benham, Lauren] Widener Univ, Dept Chem Engn, Chester, PA 19013 USA. [Chen, Jihua; Hensley, Dale K.] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. [Delaney, Kristen; Hunt, Marcus A.; Brice, Robin; Azoro, Martina] Fayetteville State Univ, Dept Biol Sci, Fayetteville, NC 28301 USA. RP Saha, D (reprint author), Widener Univ, Dept Chem Engn, Chester, PA 19013 USA. EM dsaha@mail.widener.edu RI Chen, Jihua/F-1417-2011; Hensley, Dale/A-6282-2016 OI Chen, Jihua/0000-0001-6879-5936; Hensley, Dale/0000-0001-8763-7765 FU School of Engineering of Widener University FX TEM (J.C.) and SEM (D.K.H.) experiments were conducted at the Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, which is a DOE Office of Science User Facility. D.S. acknowledges the faculty development award and provost grant from the School of Engineering of Widener University. NR 36 TC 5 Z9 5 U1 3 U2 23 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2046-2069 J9 RSC ADV JI RSC Adv. PY 2015 VL 5 IS 30 BP 23699 EP 23707 DI 10.1039/c5ra00251f PG 9 WC Chemistry, Multidisciplinary SC Chemistry GA CD6YD UT WOS:000351235800069 ER PT J AU Wu, HC Kessler, MR AF Wu, Hongchao Kessler, Michael R. TI Asphaltene: structural characterization, molecular functionalization, and application as a low-cost filler in epoxy composites SO RSC ADVANCES LA English DT Article ID NUCLEAR-MAGNETIC-RESONANCE; BORON-NITRIDE; CRUDE OILS; NANOCOMPOSITES; SPECTROSCOPY; MORPHOLOGY; POLYMERS; BEHAVIOR; BITUMEN; SURFACE AB Asphaltene obtained by extraction from asphalt was investigated by different analytical techniques in order to characterize its composition, molecular structure and morphology. Then, the asphaltene molecules were successfully functionalized by 3-glycidyloxypropyltrimethoxysilane and 3-aminopropyltriethoxysilane as confirmed by thermogravimetric analysis, X-ray photoelectron spectroscopy, and Fourier transform infrared spectroscopy. Finally, asphaltene/epoxy composites at four different loading levels were prepared and their thermo-mechanical properties were examined. The thermal analysis results indicated that asphaltene as a novel reinforcing filler in epoxy resin caused a significant increase in storage modulus of both glassy and rubbery regions, slightly increased the glass transition temperature without negatively affecting thermal stability, and reduced the overall cost of the material. C1 [Wu, Hongchao; Kessler, Michael R.] Iowa State Univ, Dept Mat Sci & Engn, Ames, IA 50011 USA. [Kessler, Michael R.] US DOE, Ames Lab, Ames, IA 50011 USA. [Kessler, Michael R.] Washington State Univ, Sch Mech & Mat Engn, Pullman, WA 99164 USA. RP Kessler, MR (reprint author), Iowa State Univ, Dept Mat Sci & Engn, Ames, IA 50011 USA. EM MichaelR.Kessler@wsu.edu RI Kessler, Michael/C-3153-2008; Wu, Hongchao/D-4808-2016 OI Kessler, Michael/0000-0001-8436-3447; Wu, Hongchao/0000-0002-0195-8398 FU Honeywell Federal Manufacturing & Technologies, LLC FX The authors acknowledge funding for this project from Honeywell Federal Manufacturing & Technologies, LLC. The authors also acknowledge Dr James Anderegg (Ames Laboratory) for his assistance with XPS measurements and Dr Steve Veysey (Department of Chemistry, Iowa State University) for his assistance with the elemental analysis. NR 43 TC 4 Z9 4 U1 7 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 2015 VL 5 IS 31 BP 24264 EP 24273 DI 10.1039/c5ra00509d PG 10 WC Chemistry, Multidisciplinary SC Chemistry GA CD6YH UT WOS:000351236300035 ER PT J AU Gillen, KT Bernstein, R Celina, M AF Gillen, K. T. Bernstein, R. Celina, M. TI CHALLENGES OF ACCELERATED AGING TECHNIQUES FOR ELASTOMER LIFETIME PREDICTIONS SO RUBBER CHEMISTRY AND TECHNOLOGY LA English DT Article ID DIFFUSION-LIMITED OXIDATION; NON-ARRHENIUS BEHAVIOR; LOW-DOSE RATE; THERMAL-OXIDATION; THEORETICAL-MODEL; TIME DEVELOPMENT; DEGRADATION; POLYETHYLENE; TEMPERATURES; PROFILES AB Elastomers are often degraded when exposed to air or high humidity for extended times (years to decades). Lifetime estimates normally involve extrapolating accelerated aging results made at higher than ambient environments. Several potential problems associated with such studies are reviewed, and experimental and theoretical methods to address them are provided. The importance of verifying time temperature superposition of degradation data is emphasized as evidence that the overall nature of the degradation process remains unchanged versus acceleration temperature. The confounding effects that occur when diffusion-limited oxidation (DLO) contributes under accelerated conditions are described, and it is shown that the DLO magnitude can be modeled by measurements or estimates of the oxygen permeability coefficient (P-Ox) and oxygen consumption rate (4)). P-Ox and phi measurements can be influenced by DLO, and it is demonstrated how confident values can be derived. In addition, several experimental profiling techniques that screen for DLO effects are discussed. Values of phi taken from high temperature to temperatures approaching ambient can be used to more confidently extrapolate accelerated aging results for air-aged materials, and many studies now show that Arrhenius extrapolations bend to lower activation energies as aging temperatures are lowered. Best approaches for accelerated aging extrapolations of humidity-exposed materials are also offered. C1 [Gillen, K. T.; Bernstein, R.; Celina, M.] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Gillen, KT (reprint author), Sandia Natl Labs, Box 5800, Albuquerque, NM 87185 USA. EM dandkgillen@comcast.net FU U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX Sandia National Laboratories is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000. NR 36 TC 0 Z9 0 U1 8 U2 29 PU AMER CHEMICAL SOC INC PI AKRON PA RUBBER DIV UNIV AKRON PO BOX 499, AKRON, OH 44309-0499 USA SN 0035-9475 EI 1943-4804 J9 RUBBER CHEM TECHNOL JI Rubber Chem. Technol. PD JAN-MAR PY 2015 VL 88 IS 1 BP 1 EP 27 DI 10.5254/rct.14.85930 PG 27 WC Polymer Science SC Polymer Science GA CE2MD UT WOS:000351648800001 ER PT J AU Liu, AJ Grest, GS Marchetti, MC Grason, GM Robbins, MO Fredrickson, GH Rubinstein, M de la Cruz, MO AF Liu, Andrea J. Grest, Gary S. Marchetti, M. Cristina Grason, Gregory M. Robbins, Mark O. Fredrickson, Glenn H. Rubinstein, Michael de la Cruz, Monica Olvera TI Opportunities in theoretical and computational polymeric materials and soft matter SO SOFT MATTER LA English DT Article AB Soft materials are abundant in nature and ubiquitous in living systems. Elucidating their multi-faceted properties and underlying mechanisms is not only theoretically challenging and important in its own right, but also serves as the foundation for new materials and applications that will have wide-ranging impact on technology and the national economy. Recent initiatives in computation and data-driven materials discovery, such as the Materials Genome Initiative and the National Science Foundation Designing Materials to Revolutionize and Engineer our Future (NSF-DMREF) program, recognize and highlight the many future opportunities in the field. Building upon similar past efforts, a workshop was held at the University of California, Santa Barbara in October 2013 to specifically identify the central challenges and opportunities in theoretical and computational studies of polymeric as well as non-polymeric soft materials. This article presents a summary of the main findings of the workshop. C1 [Liu, Andrea J.] Univ Penn, Dept Phys & Astron, Philadelphia, PA 19014 USA. [Grest, Gary S.] Sandia Natl Labs, Ctr Integrated Nanotechnol, Albuquerque, NM 87185 USA. [Marchetti, M. Cristina] Syracuse Univ, Dept Phys, Syracuse, NY 13244 USA. [Marchetti, M. Cristina] Syracuse Univ, Syracuse Biomat Inst, Syracuse, NY 13244 USA. [Grason, Gregory M.] Univ Massachusetts, Dept Polymer Sci & Engn, Amherst, MA 01003 USA. [Robbins, Mark O.] Johns Hopkins Univ, Dept Phys & Astron, Baltimore, MD 21218 USA. [Fredrickson, Glenn H.] Univ Calif Santa Barbara, Dept Chem Engn, Santa Barbara, CA 93106 USA. [Fredrickson, Glenn H.] Univ Calif Santa Barbara, Dept Mat, Santa Barbara, CA 93106 USA. [Fredrickson, Glenn H.] Univ Calif Santa Barbara, Mat Res Lab, Santa Barbara, CA 93106 USA. [Rubinstein, Michael] Univ N Carolina, Dept Chem, Chapel Hill, NC 27599 USA. [de la Cruz, Monica Olvera] Northwestern Univ, Dept Mat Sci & Engn, Evanston, IL 60208 USA. RP Rubinstein, M (reprint author), Univ N Carolina, Dept Chem, Chapel Hill, NC 27599 USA. FU NSF FX This article summarizes the report that can be downloaded at http://www.nsfreport.polymericso.materials.northwestern.edu/final_report .pdf, which is the result of hard work by all workshop participants, and we would like to thank them for their cooperation and wisdom during the two and a half days of the workshop. We are especially grateful to Drs. Mark Bowick, Alexander Grosberg, Sanat Kumar, Sharon Glotzer, Fred MacKintosh, Murugappan Muthukumar, Kenneth Shull, Dvora Perahia and Thomas Witten who made an extra effort to write summaries of the discussions of the working groups and to edit the corresponding parts of the report, and to Ting Ge for designing the cover of the report. We thank William Kung at the NU-MRSEC for input in the organization and editing of both the article and the report and to Sara Bard and Naomi Recania of UCSB for their superb local orchestration of the workshop. Finally, we would like to thank NSF for funding the workshop and CMMT Program directors Drs. Daryl Hess and Andrey Dobrynin for their support and assistance throughout the whole process. NR 5 TC 7 Z9 7 U1 9 U2 74 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1744-683X EI 1744-6848 J9 SOFT MATTER JI Soft Matter PY 2015 VL 11 IS 12 BP 2326 EP 2332 DI 10.1039/c4sm02344g PG 7 WC Chemistry, Physical; Materials Science, Multidisciplinary; Physics, Multidisciplinary; Polymer Science SC Chemistry; Materials Science; Physics; Polymer Science GA CD9DC UT WOS:000351396500001 PM 25711605 ER PT J AU Ingham, B Erlangga, GD Smialowska, A Kirby, NM Wang, C Matia-Merino, L Haverkamp, RG Carr, AJ AF Ingham, B. Erlangga, G. D. Smialowska, A. Kirby, N. M. Wang, C. Matia-Merino, L. Haverkamp, R. G. Carr, A. J. TI Solving the mystery of the internal structure of casein micelles SO SOFT MATTER LA English DT Article ID ANGLE NEUTRON-SCATTERING; X-RAY-SCATTERING; SUB-MICELLES; FILTRATION; MODEL; MILK AB The interpretation ofmilk X-ray and neutron scattering data in relation to the internal structure of the casein micelle is an ongoing debate. We performed resonant X-ray scattering measurements on liquid milk and conclusively identified key scattering features, namely those corresponding to the size of and the distance between colloidal calcium phosphate particles. An X-ray scattering feature commonly assigned to the particle size is instead due to protein inhomogeneities. C1 [Ingham, B.] Callaghan Innovat, Lower Hutt 5040, New Zealand. [Ingham, B.] Victoria Univ Wellington, MacDiarmid Inst Adv Mat & Nanotechnol, Wellington 6140, New Zealand. [Erlangga, G. D.; Smialowska, A.; Matia-Merino, L.; Carr, A. J.] Massey Univ, Sch Food & Nutr, Palmerston North 4442, New Zealand. [Kirby, N. M.] Australian Synchrotron, Clayton, Vic 3168, Australia. [Wang, C.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. [Haverkamp, R. G.] Massey Univ, Sch Engn & Adv Technol, Palmerston North 4442, New Zealand. RP Ingham, B (reprint author), Callaghan Innovat, POB 31-310, Lower Hutt 5040, New Zealand. EM bridget.ingham@callaghaninnovation.govt.nz; a.j.carr@massey.ac.nz RI Haverkamp, Richard/H-1149-2012; Wang, Cheng/A-9815-2014; Carr, Alistair/S-6016-2016 OI Haverkamp, Richard/0000-0002-3890-7105; Carr, Alistair/0000-0003-4545-3014 FU New Zealand Ministry of Business, Innovation and Employment (MBIE) [C08X1003]; Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231] FX This work was funded by the New Zealand Ministry of Business, Innovation and Employment (MBIE) under contract C08X1003. Portions of this research were undertaken on the SAXS/WAXS beamline at the Australian Synchrotron, Victoria, Australia, and beamline 11.0.1 at the Advanced Light Source, Berkeley. 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 32 TC 7 Z9 7 U1 8 U2 53 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1744-683X EI 1744-6848 J9 SOFT MATTER JI Soft Matter PY 2015 VL 11 IS 14 BP 2723 EP 2725 DI 10.1039/c5sm00153f PG 3 WC Chemistry, Physical; Materials Science, Multidisciplinary; Physics, Multidisciplinary; Polymer Science SC Chemistry; Materials Science; Physics; Polymer Science GA CE3FK UT WOS:000351711800002 PM 25711160 ER PT J AU Sun, Y Tsuchiya, Y Pyon, S Tamegai, T Zhang, C Ozaki, T Li, Q AF Sun, Yue Tsuchiya, Yuji Pyon, Sunseng Tamegai, Tsuyoshi Zhang, Cheng Ozaki, Toshinori Li, Qiang TI Magneto-optical characterizations of FeTe0.5Se0.5 thin films with critical current density over 1 MA cm(-2) SO SUPERCONDUCTOR SCIENCE & TECHNOLOGY LA English DT Article DE iron-based superconductors; thin film; Magneto-optical imaging ID SINGLE-CRYSTAL; SUPERCONDUCTORS AB We performed magneto-optical (MO) measurements on FeTe0.5Se0.5 thin films grown on LaAlO3 (LAO) and Yttria-stabilized zirconia (YSZ) single-crystalline substrates. These thin films show superconducting transition temperature T-c similar to 19 K, 4 K higher than the bulk sample. Typical roof-top patterns can be observed in the MO images of thin films grown on LAO and YSZ, from which a large and homogeneous critical current density J(c) over 1 x 10(6) A cm(-2) at 5 K was obtained. Magnetic flux penetration measurement reveals that the current is almost isotropically distributed in the two thin films. Compared with bulk crystals, FeTe0.5Se0.5 thin film demonstrates not only higher T-c, but also much larger J(c), which is attractive for applications. C1 [Sun, Yue; Tsuchiya, Yuji; Pyon, Sunseng; Tamegai, Tsuyoshi] Univ Tokyo, Dept Appl Phys, Bunkyo Ku, Tokyo 1138656, Japan. [Zhang, Cheng; Ozaki, Toshinori; Li, Qiang] Brookhaven Natl Lab, Condensed Matter Phys & Mat Sci Dept, Upton, NY 11973 USA. RP Sun, Y (reprint author), Univ Tokyo, Dept Appl Phys, Bunkyo Ku, 7-3-1 Hongo, Tokyo 1138656, Japan. EM sunyue.seu@gmail.com RI 悦, 孙/B-1373-2013; Zhang, Cheng/R-6593-2016 OI 悦, 孙/0000-0002-5189-5460; Zhang, Cheng/0000-0001-6531-4703 FU Japan Society for the Promotion of Science; Japan-China Bilateral Joint Research Project of the Japan Society for the Promotion of Science; U.S. Department of Energy, Office of Basic Energy Science, Materials Sciences and Engineering Division [DEAC0298CH10886] FX Yue Sun gratefully appreciates the support from the Japan Society for the Promotion of Science. The work at the University of Tokyo was supported by the Japan-China Bilateral Joint Research Project of the Japan Society for the Promotion of Science. The work at Brookhaven National Laboratory was supported by the U.S. Department of Energy, Office of Basic Energy Science, Materials Sciences and Engineering Division, under contract no. DEAC0298CH10886. NR 31 TC 7 Z9 7 U1 3 U2 17 PU IOP PUBLISHING LTD PI BRISTOL PA TEMPLE CIRCUS, TEMPLE WAY, BRISTOL BS1 6BE, ENGLAND SN 0953-2048 EI 1361-6668 J9 SUPERCOND SCI TECH JI Supercond. Sci. Technol. PD JAN PY 2015 VL 28 IS 1 AR 015010 DI 10.1088/0953-2048/28/1/015010 PG 6 WC Physics, Applied; Physics, Condensed Matter SC Physics GA CD3QJ UT WOS:000350994100018 ER PT J AU Labios, LA Weiss, CJ Egbert, JD Lense, S Bullock, RM Dougherty, WG Kassel, WS Mock, MT AF Labios, Liezel A. Weiss, Charles J. Egbert, Jonathan D. Lense, Sheri Bullock, R. Morris Dougherty, William G. Kassel, W. Scott Mock, Michael T. TI Synthesis and Protonation Studies of Molybdenum(0) Bis(dinitrogen) Complexes Supported by Diphosphine Ligands Containing Pendant Amines SO ZEITSCHRIFT FUR ANORGANISCHE UND ALLGEMEINE CHEMIE LA English DT Article DE Nitrogen fixation; Molybdenum; Diphosphine ligands; Dinitrogen complex; Proton relay ID DINITROGEN COMPLEXES; TUNGSTEN-DINITROGEN; NITROGEN-FIXATION; AMMONIA; CHEMISTRY; IRON; COORDINATION; REDUCTION; MECHANISM; TETRAHYDROFURAN AB A series of molybdenum bis(dinitrogen) complexes of the formula trans-[Mo(N-2)(2)((PNPEt)-N-Et-P-R)(2)] ((PNPEt)-N-Et-P-R = Et2PCH2N(R)CH2PEt2; R = phenyl (1), 2,6-difluorobenzyl (2), 3,5-difluorobenzyl (3), CH2CH2NMe2 (4), CH2-o-Py (5)] were synthesized and characterized by NMR and IR spectroscopy, and X-ray crystallography. Protonation studies with stoichiometric amounts of triflic acid (HOTf) were performed, and the protonated products were characterized by NMR and in situ IR spectroscopic methods. Products formed in the stepwise protonation reactions included, for example, a mixture of the seven-coordinate molybdenum bis(dinitrogen) hydride, trans-[Mo(H)(N-2)(2)((PNPEt)-N-Et-P-Ph)(2)](+) [H-1](+), and the Mo-hydrazido triflate complex, trans-[Mo(NNH2)(OTf)((PNPEt)-N-Et-P-Ph)(2)](+) [(1)(NNH2)](+). Complex 2, with more basic pendant amines, can be protonated up to three times, affording the highly-charged molecule, trans[Mo(H)(N-2)(2)((PN2,6-F2-Bn)-N-Et(H)P-Et)(2))](3+) [2H(PN(H)P)(2)](3+). C1 [Labios, Liezel A.; Weiss, Charles J.; Egbert, Jonathan D.; Lense, Sheri; Bullock, R. Morris; Mock, Michael T.] Pacific NW Natl Lab, Ctr Mol Electrocatalysis, Div Phys Sci, Richland, WA 99352 USA. [Dougherty, William G.; Kassel, W. Scott] Villanova Univ, Dept Chem, Villanova, PA 19085 USA. RP Mock, MT (reprint author), Pacific NW Natl Lab, Ctr Mol Electrocatalysis, Div Phys Sci, POB 999, Richland, WA 99352 USA. EM michael.mock@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; DOE Office of Science, Early Career Research Program through the Office of Basic Energy Sciences FX This work 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. S. L. was supported by the DOE Office of Science, Early Career Research Program through the Office of Basic Energy Sciences. Pacific Northwest National Laboratory is operated by Battelle for the DOE. NR 53 TC 6 Z9 6 U1 2 U2 18 PU WILEY-V C H VERLAG GMBH PI WEINHEIM PA BOSCHSTRASSE 12, D-69469 WEINHEIM, GERMANY SN 0044-2313 EI 1521-3749 J9 Z ANORG ALLG CHEM JI Z. Anorg. Allg. Chem. PD JAN PY 2015 VL 641 IS 1 SI SI BP 105 EP 117 DI 10.1002/zaac.201400119 PG 13 WC Chemistry, Inorganic & Nuclear SC Chemistry GA CD9TZ UT WOS:000351442700017 ER PT J AU Cunsolo, A AF Cunsolo, Alessandro TI The THz Spectrum of Density Fluctuations of Water: The Viscoelastic Regime SO ADVANCES IN CONDENSED MATTER PHYSICS LA English DT Review ID X-RAY-SCATTERING; WAVELENGTH COLLECTIVE EXCITATIONS; INELASTIC NEUTRON-SCATTERING; LENNARD-JONES FLUIDS; SUPERCOOLED WATER; LIQUID WATER; BRILLOUIN-SCATTERING; MOLECULAR-DYNAMICS; SOUND-VELOCITY; STRUCTURAL RELAXATION AB Relevant advances in the knowledge of the water dynamics at mesoscopic scales are reviewed, while mainly focusing on the contribution provided by high resolution inelastic X-ray scattering (IXS). In particular it is discussed how the use of IXS has improved our understanding of viscoelastic properties of water at THz frequencies. This specifically involves some solid-like features such as the onset of shear wave propagation, a sound velocity surprisingly similar to the one of ice, and an anomalously low sound absorption coefficient. All these properties can be explained by assuming the coupling of THz density fluctuations with a structural relaxation process connected to the breaking and forming of hydrogen bonds (HBs). This review also includes more recent IXS results demonstrating that, upon approaching supercritical conditions, relaxation phenomena in water gradually lose their structural character becoming essentially collisional in character. Furthermore, GHz spectroscopy results on supercooled water, suggesting the occurrence of a structural arrest, are discussed. An overview of the new opportunities offered by next generation IXS spectrometers finally concludes this review. C1 Brookhaven Natl Lab, Photon Sci Directorate, Upton, NY 11973 USA. RP Cunsolo, A (reprint author), Brookhaven Natl Lab, Photon Sci Directorate, POB 5000, Upton, NY 11973 USA. EM acunsolo@bnl.gov NR 115 TC 2 Z9 2 U1 4 U2 31 PU HINDAWI PUBLISHING CORP PI NEW YORK PA 410 PARK AVENUE, 15TH FLOOR, #287 PMB, NEW YORK, NY 10022 USA SN 1687-8108 EI 1687-8124 J9 ADV COND MATTER PHYS JI Adv. Condens. Matter Phys. PY 2015 AR 137435 DI 10.1155/2015/137435 PG 24 WC Physics, Condensed Matter SC Physics GA CD4PD UT WOS:000351064800001 ER PT S AU Bauer, ED Thompson, JD AF Bauer, E. D. Thompson, J. D. BE Langer, JS TI Plutonium-Based Heavy-Fermion Systems SO ANNUAL REVIEW OF CONDENSED MATTER PHYSICS, VOL 6 SE Annual Review of Condensed Matter Physics LA English DT Review; Book Chapter DE Kondo effect; mixed valence; hybridization; unconventional superconductivity; magnetism; spin fluctuations; charge fluctuations; quasiparticles ID SINGLE-CRYSTAL GROWTH; UNCONVENTIONAL SUPERCONDUCTIVITY; UNIVERSAL RELATIONSHIP; MAGNETIC-RESONANCE; ELECTRON SYSTEMS; ACTINIDE METALS; 5F ORBITALS; SPECTROSCOPY; STATES; INTERMETALLICS AB An effective mass of charge carriers that is significantly larger than the mass of a free electron develops at low temperatures in certain lanthanide- and actinide-based metals, including those formed with plutonium, owing to strong electron-electron interactions. This heavy-fermion mass is reflected in a substantially enhanced electronic coefficient of specific heat gamma, which for elemental Pu is much larger than that of normal metals. By our definition, there are twelve Pu-based heavy-fermion compounds, most discovered recently, whose basic properties are known and discussed. Relative to other examples, these Pu-based heavy-fermion systems are particularly complex owing in part to the possible simultaneous presence of multiple, nearly degenerate 5f(n) configurations. This complexity poses significant opportunities as well as challenges, including understanding the origin of unconventional superconductivity in some of these materials. C1 [Bauer, E. D.; Thompson, J. D.] Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Thompson, JD (reprint author), Los Alamos Natl Lab, POB 1663, Los Alamos, NM 87545 USA. EM edbauer@lanl.gov; jdt@lanl.gov OI Bauer, Eric/0000-0003-0017-1937 NR 74 TC 3 Z9 3 U1 6 U2 20 PU ANNUAL REVIEWS PI PALO ALTO PA 4139 EL CAMINO WAY, PO BOX 10139, PALO ALTO, CA 94303-0897 USA SN 1947-5454 BN 978-0-8243-5006-2 J9 ANNU REV CONDEN MA P JI Annu. Rev. Condens. Matter Phys. PY 2015 VL 6 BP 137 EP 153 DI 10.1146/annurev-conmatphys-031214-014508 PG 17 WC Physics, Condensed Matter SC Physics GA BC2IQ UT WOS:000350979900007 ER PT J AU Hess, P Kinnison, D Tang, Q AF Hess, P. Kinnison, D. Tang, Q. TI Ensemble simulations of the role of the stratosphere in the attribution of northern extratropical tropospheric ozone variability SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID ATMOSPHERIC RESEARCH STATION; NINO SOUTHERN-OSCILLATION; LONG-TERM CHANGES; MACE-HEAD; SURFACE OZONE; INTERANNUAL VARIABILITY; SEASONAL VARIABILITY; MOZAIC PROGRAM; AIR-POLLUTION; CLIMATE AB Despite the need to understand the impact of changes in emissions and climate on tropospheric ozone, the attribution of tropospheric interannual ozone variability to specific processes has proven difficult. Here, we analyze the stratospheric contribution to tropospheric ozone variability and trends from 1953 to 2005 in the Northern Hemisphere (NH) mid-latitudes using four ensemble simulations of the free running (FR) Whole Atmosphere Community Climate Model (WACCM). The simulations are externally forced with observed time-varying (1) sea-surface temperatures (SSTs), (2) greenhouse gases (GHGs), (3) ozone depleting substances (ODS), (4) quasi-biennial oscillation (QBO), (5) solar variability (SV) and (6) stratospheric sulfate surface area density (SAD). A detailed representation of stratospheric chemistry is simulated, including the ozone loss due to volcanic eruptions and polar stratospheric clouds. In the troposphere, ozone production is represented by CH4-NOx smog chemistry, where surface chemical emissions remain interannually constant. Despite the simplicity of its tropospheric chemistry, at many NH measurement locations, the interannual ozone variability in the FR WACCM simulations is significantly correlated with the measured interannual variability. This suggests the importance of the external forcing applied in these simulations in driving interannual ozone variability. The variability and trend in the simulated 1953-2005 tropospheric ozone from 30 to 90 degrees N at background surface measurement sites, 500 hPa measurement sites and in the area average are largely explained on interannual timescales by changes in the 30-90 degrees N area averaged flux of ozone across the 100 hPa surface and changes in tropospheric methane concentrations. The average sensitivity of tropospheric ozone to methane (percent change in ozone to a percent change in methane) from 30 to 90 degrees N is 0.17 at 500 hPa and 0.21 at the surface; the average sensitivity of tropospheric ozone to the 100 hPa ozone flux (percent change in ozone to a percent change in the ozone flux) from 30 to 90 degrees N is 0.19 at 500 hPa and 0.11 at the surface. The 30-90 degrees N simulated downward residual velocity at 100 hPa increased by 15% between 1953 and 2005. However, the impact of this on the 30-90 degrees N 100 hPa ozone flux is modulated by the long-term changes in stratospheric ozone. The ozone flux decreases from 1965 to 1990 due to stratospheric ozone depletion, but increases again by approximately 7% from 1990 to 2005. The first empirical orthogonal function of interannual ozone variability explains from 40% (at the surface) to over 80% (at 150 hPa) of the simulated ozone interannual variability from 30 to 90 degrees N. This identified mode of ozone variability shows strong stratosphere-troposphere coupling, demonstrating the importance of the stratosphere in an attribution of tropospheric ozone variability. The simulations, with no change in emissions, capture almost 50% of the measured ozone change during the 1990s at a variety of locations. This suggests that a large portion of the measured change is not due to changes in emissions, but can be traced to changes in large-scale modes of ozone variability. This emphasizes the difficulty in the attribution of ozone changes, and the importance of natural variability in understanding the trends and variability of ozone. We find little relation between the El Nino-Southern Oscillation (ENSO) index and large-scale tropospheric ozone variability over the long-term record. C1 [Hess, P.] Cornell Univ, Dept Biol & Environm Engn, Ithaca, NY 14850 USA. [Kinnison, D.] Natl Ctr Atmospher Res, Boulder, CO 80307 USA. [Tang, Q.] Lawrence Livermore Natl Lab, Livermore, CA USA. RP Hess, P (reprint author), Cornell Univ, Dept Biol & Environm Engn, Ithaca, NY 14850 USA. EM pgh25@cornell.edu RI Tang, Qi/C-1032-2011; Hess, Peter/M-3145-2015 OI Hess, Peter/0000-0003-2439-3796 FU NSF [1042787]; US Department of Energy (DOE), Office of Science, Office of Biological and Environmental Research by Lawrence Livermore National Laboratory [DE-AC52-07NA27344]; Atmospheric Radiation Measurement Program of the Office of Science at the US Department of Energy; National Science Foundation; US Department of Energy FX The authors would like to thank the reviewers for their helpful comments. P. G. Hess would like to acknowledge NSF grant no. 1042787 for supporting this work. Work at LLNL was performed under the auspices of the US Department of Energy (DOE), Office of Science, Office of Biological and Environmental Research by Lawrence Livermore National Laboratory under contract DE-AC52-07NA27344 and supported by the Atmospheric Radiation Measurement Program of the Office of Science at the US Department of Energy. The CESM project is supported by the National Science Foundation and 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. We acknowledge the World Ozone and Ultraviolet Radiation Data Centre (WOUDC) for providing the ozonesonde data, the US National Park Service for providing Lassen NP ozone data, A. Volz-Thomas for the Arkona data, and D. Parrish for providing access to his surface composited ozone data sets. NR 77 TC 7 Z9 7 U1 3 U2 13 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1680-7316 EI 1680-7324 J9 ATMOS CHEM PHYS JI Atmos. Chem. Phys. PY 2015 VL 15 IS 5 BP 2341 EP 2365 DI 10.5194/acp-15-2341-2015 PG 25 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA CC7PE UT WOS:000350559700007 ER PT J AU Hiranuma, N Augustin-Bauditz, S Bingemer, H Budke, C Curtius, J Danielczok, A Diehl, K Dreischmeier, K Ebert, M Frank, F Hoffmann, N Kandler, K Kiselev, A Koop, T Leisner, T Mohler, O Nillius, B Peckhaus, A Rose, D Weinbruch, S Wex, H Boose, Y DeMott, PJ Hader, JD Hill, TCJ Kanji, ZA Kulkarni, G Levin, EJT McCluskey, CS Murakami, M Murray, BJ Niedermeier, D Petters, MD O'Sullivan, D Saito, A Schill, GP Tajiri, T Tolbert, MA Welti, A Whale, TF Wright, TP Yamashita, K AF Hiranuma, N. Augustin-Bauditz, S. Bingemer, H. Budke, C. Curtius, J. Danielczok, A. Diehl, K. Dreischmeier, K. Ebert, M. Frank, F. Hoffmann, N. Kandler, K. Kiselev, A. Koop, T. Leisner, T. Moehler, O. Nillius, B. Peckhaus, A. Rose, D. Weinbruch, S. Wex, H. Boose, Y. DeMott, P. J. Hader, J. D. Hill, T. C. J. Kanji, Z. A. Kulkarni, G. Levin, E. J. T. McCluskey, C. S. Murakami, M. Murray, B. J. Niedermeier, D. Petters, M. D. O'Sullivan, D. Saito, A. Schill, G. P. Tajiri, T. Tolbert, M. A. Welti, A. Whale, T. F. Wright, T. P. Yamashita, K. TI A comprehensive laboratory study on the immersion freezing behavior of illite NX particles: a comparison of 17 ice nucleation measurement techniques SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID MINERAL DUST AEROSOL; FLOW DIFFUSION CHAMBER; KAOLINITE PARTICLES; DEPOSITION NUCLEATION; CRYSTAL NUCLEATION; HEMATITE PARTICLES; WATER DROPLETS; WIND-TUNNEL; NUCLEI; MODE AB Immersion freezing is the most relevant heterogeneous ice nucleation mechanism through which ice crystals are formed in mixed-phase clouds. In recent years, an increasing number of laboratory experiments utilizing a variety of instruments have examined immersion freezing activity of atmospherically relevant ice-nucleating particles. However, an intercomparison of these laboratory results is a difficult task because investigators have used different ice nucleation (IN) measurement methods to produce these results. A remaining challenge is to explore the sensitivity and accuracy of these techniques and to understand how the IN results are potentially influenced or biased by experimental parameters associated with these techniques. Within the framework of INUIT (Ice Nuclei Research Unit), we distributed an illite-rich sample (illite NX) as a representative surrogate for atmospheric mineral dust particles to investigators to perform immersion freezing experiments using different IN measurement methods and to obtain IN data as a function of particle concentration, temperature (T), cooling rate and nucleation time. A total of 17 measurement methods were involved in the data intercomparison. Experiments with seven instruments started with the test sample pre-suspended in water before cooling, while 10 other instruments employed water vapor condensation onto dry-dispersed particles followed by immersion freezing. The resulting comprehensive immersion freezing data set was evaluated using the ice nucleation active surface-site density, n(s), to develop a representative n(s)(T) spectrum that spans a wide temperature range (-37 degrees C < T < -11 degrees C) and covers 9 orders of magnitude in n(s). In general, the 17 immersion freezing measurement techniques deviate, within a range of about 8 degrees C in terms of temperature, by 3 orders of magnitude with respect to n(s). In addition, we show evidence that the immersion freezing efficiency expressed in n(s) of illite NX particles is relatively independent of droplet size, particle mass in suspension, particle size and cooling rate during freezing. A strong temperature dependence and weak time and size dependence of the immersion freezing efficiency of illite-rich clay mineral particles enabled the n(s) parameterization solely as a function of temperature. We also characterized the n(s)(T) spectra and identified a section with a steep slope between -20 and -27 degrees C, where a large fraction of active sites of our test dust may trigger immersion freezing. This slope was followed by a region with a gentler slope at temperatures below -27 degrees C. While the agreement between different instruments was reasonable below similar to -27 degrees C, there seemed to be a different trend in the temperature-dependent ice nucleation activity from the suspension and dry-dispersed particle measurements for this mineral dust, in particular at higher temperatures. For instance, the ice nucleation activity expressed in n(s) was smaller for the average of the wet suspended samples and higher for the average of the dry-dispersed aerosol samples between about -27 and -18 degrees C. Only instruments making measurements with wet suspended samples were able to measure ice nucleation above -18 degrees C. A possible explanation for the deviation between -27 and -18 degrees C is discussed. Multiple exponential distribution fits in both linear and log space for both specific surface area-based n(s)(T) and geometric surface area-based n(s)(T) are provided. These new fits, constrained by using identical reference samples, will help to compare IN measurement methods that are not included in the present study and IN data from future IN instruments. C1 [Hiranuma, N.; Hoffmann, N.; Kiselev, A.; Leisner, T.; Moehler, O.; Peckhaus, A.] Karlsruhe Inst Technol, Inst Meteorol & Climate Res Atmospher Aerosol Res, D-76021 Karlsruhe, Germany. [Augustin-Bauditz, S.; Wex, H.; Niedermeier, D.] Leibniz Inst Tropospher Res, Leipzig, Germany. [Bingemer, H.; Curtius, J.; Danielczok, A.; Frank, F.; Nillius, B.; Rose, D.] Goethe Univ Frankfurt, Inst Atmospher & Environm Sci, D-60054 Frankfurt, Germany. [Budke, C.; Dreischmeier, K.; Koop, T.] Univ Bielefeld, Fac Chem, Bielefeld, Germany. [Diehl, K.] Johannes Gutenberg Univ Mainz, Inst Atmospher Phys, D-55122 Mainz, Germany. [Ebert, M.; Kandler, K.; Weinbruch, S.] Tech Univ Darmstadt, Inst Appl Geosci, Darmstadt, Germany. [Boose, Y.; Kanji, Z. A.; Welti, A.] ETH, Inst Atmosphere & Climate Sci, Zurich, Switzerland. [DeMott, P. J.; Hill, T. C. J.; Levin, E. J. T.; McCluskey, C. S.] Colorado State Univ, Dept Atmospher Sci, Ft Collins, CO 80523 USA. [Hader, J. D.; Petters, M. D.; Wright, T. P.] N Carolina State Univ, Dept Marine Earth & Atmospher Sci, Raleigh, NC 27695 USA. [Kulkarni, G.] Pacific NW Natl Lab, Atmospher Sci & Global Change Div, Richland, WA 99352 USA. [Murakami, M.; Saito, A.; Tajiri, T.; Yamashita, K.] Meteorol Res Inst, Tsukuba, Ibaraki 305, Japan. [Murray, B. J.; O'Sullivan, D.; Whale, T. F.] Univ Leeds, Sch Earth & Environm, Inst Climate & Atmospher Sci, Leeds, W Yorkshire, England. [Schill, G. P.; Tolbert, M. A.] Univ Colorado, Cooperat Inst Res Environm Sci, Boulder, CO 80309 USA. [Schill, G. P.; Tolbert, M. A.] Univ Colorado, Dept Chem & Biochem, Boulder, CO 80309 USA. RP Hiranuma, N (reprint author), Karlsruhe Inst Technol, Inst Meteorol & Climate Res Atmospher Aerosol Res, D-76021 Karlsruhe, Germany. EM seong.moon@kit.edu RI Curtius, Joachim/A-2681-2011; Kiselev, Alexei/A-3036-2013; Koop, Thomas/B-7861-2008; Murray, Benjamin/C-1219-2010; Levin, Ezra/F-5809-2010; Weinbruch, Stephan/E-6141-2014; Hiranuma, Naruki/D-3780-2014; DeMott, Paul/C-4389-2011; Schill, Gregory/J-4031-2015; Petters, Markus/D-2144-2009; O'Sullivan, Daniel/G-3884-2012; Mohler, Ottmar/J-9426-2012; Kandler, Konrad/C-3467-2014; Leisner, Thomas/A-2391-2013; OI Curtius, Joachim/0000-0003-3153-4630; Kiselev, Alexei/0000-0003-0136-2428; Koop, Thomas/0000-0002-7571-3684; Murray, Benjamin/0000-0002-8198-8131; Hiranuma, Naruki/0000-0001-7790-4807; DeMott, Paul/0000-0002-3719-1889; Schill, Gregory/0000-0002-4084-0317; Petters, Markus/0000-0002-4082-1693; O'Sullivan, Daniel/0000-0002-6884-8046; Kanji, Zamin/0000-0001-8610-3921 FU Deutsche Forschungsgemeinschaft (DFG) within Research Unit FOR 1525 (INUIT) [BU 1432/4-1, DI 1539/1-1, KO2944/2-1, MO668/4-1, WE 4722/1-1]; Deutsche Forschungsgemeinschaft; Open Access Publishing Fund of Karlsruhe Institute of Technology; Department of Energy (DOE) Atmospheric System Research Program; DOE [DE-AC05-76RLO 1830]; Swiss National Funds; NSF [AGS-1358495, AGS 1048536, AGS 1010851]; JSPS KAKENHI [23244095]; Natural Environment Research Council [NE/K004417/1, NE/I020059/1, NE/I013466/1, NE/I019057/1]; European Research Council [240449 - ICE]; Alexander von Humboldt-foundation, Germany FX Part of this work is funded by Deutsche Forschungsgemeinschaft (DFG) under contracts BU 1432/4-1, DI 1539/1-1, KO2944/2-1, MO668/4-1 and WE 4722/1-1 within Research Unit FOR 1525 (INUIT). The authors acknowledge partial financial support by Deutsche Forschungsgemeinschaft and Open Access Publishing Fund of Karlsruhe Institute of Technology. The authors gratefully acknowledge skillful and continuous support from their technical teams. G. Kulkarni acknowledges support from the Department of Energy (DOE) Atmospheric System Research Program and thanks J. Fast for useful discussion. Battelle Memorial Institute operates the Pacific Northwest National Laboratory for DOE under contract DE-AC05-76RLO 1830. Z. A. Kanji acknowledges funding from Swiss National Funds. P. J. DeMott and T. Hill were funded by NSF grant award number AGS-1358495. M. A. Tolbert and G. P. Schill were funded by NSF Grant AGS 1048536. The MRI-DCECC work was partly funded by JSPS KAKENHI Grant Numbers 23244095. T. P. Wright, J. D. Hader, and M. D. Petters were funded by NSF Grant AGS 1010851. B. J. Murray, D. O'Sullivan and T. F. Whale acknowledge the Natural Environment Research Council (NE/K004417/1; NE/I020059/1; NE/I013466/1; NE/I019057/1) and The European Research Council (240449 - ICE) for funding. D. Niedermeier acknowledges financial support from the Alexander von Humboldt-foundation, Germany. NR 105 TC 37 Z9 37 U1 9 U2 65 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1680-7316 EI 1680-7324 J9 ATMOS CHEM PHYS JI Atmos. Chem. Phys. PY 2015 VL 15 IS 5 BP 2489 EP 2518 DI 10.5194/acp-15-2489-2015 PG 30 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA CC7PE UT WOS:000350559700016 ER PT J AU Ahn, MH Han, D Won, HY Morris, V AF Ahn, M. -H. Han, D. Won, H. Y. Morris, V. TI A cloud detection algorithm using the downwelling infrared radiance measured by an infrared pyrometer of the ground-based microwave radiometer SO ATMOSPHERIC MEASUREMENT TECHNIQUES LA English DT Article ID SOUTHERN GREAT-PLAINS; LIQUID WATER PATH; RADIATION; VAPOR; TEMPERATURE; SKIES; CLEAR; SKY; RETRIEVAL; EQUATIONS AB For better utilization of the ground-based microwave radiometer, it is important to detect the cloud presence in the measured data. Here, we introduce a simple and fast cloud detection algorithm by using the optical characteristics of the clouds in the infrared atmospheric window region. The new algorithm utilizes the brightness temperature (Tb) measured by an infrared radiometer installed on top of a microwave radiometer. The two-step algorithm consists of a spectral test followed by a temporal test. The measured Tb is first compared with a predicted clear-sky Tb obtained by an empirical formula as a function of surface air temperature and water vapor pressure. For the temporal test, the temporal variability of the measured Tb during one minute compares with a dynamic threshold value, representing the variability of clear-sky conditions. It is designated as cloudfree data only when both the spectral and temporal tests confirm cloud-free data. Overall, most of the thick and uniform clouds are successfully detected by the spectral test, while the broken and fast-varying clouds are detected by the temporal test. The algorithm is validated by comparison with the collocated ceilometer data for six months, from January to June 2013. The overall proportion of correctness is about 88.3% and the probability of detection is 90.8 %, which are comparable with or better than those of previous similar approaches. Two thirds of discrepancies occur when the new algorithm detects clouds while the ceilometer does not, resulting in different values of the probability of detection with different cloud-base altitude, 93.8, 90.3, and 82.8% for low, mid, and high clouds, respectively. Finally, due to the characteristics of the spectral range, the new algorithm is found to be insensitive to the presence of inversion layers. C1 [Ahn, M. -H.; Han, D.; Won, H. Y.] Ewha Womans Univ, Dept Atmospher Sci & Engn, Seoul, South Korea. [Morris, V.] Pacific NW Natl Lab, Richland, WA 99352 USA. RP Ahn, MH (reprint author), Ewha Womans Univ, Dept Atmospher Sci & Engn, Ewha Yeodae Gil 52, Seoul, South Korea. EM terryahn65@ewha.ac.kr FU National Institute of Meteorological Research (NIMR) [NIMR-2012-B-1] FX This work is supported by the "Development and application of technology for weather forecasting (NIMR-2012-B-1)" of the National Institute of Meteorological Research (NIMR). The authors are grateful to the KMA for providing the radiometer, ceilometer, and ground observation data. NR 36 TC 2 Z9 2 U1 2 U2 7 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 2015 VL 8 IS 2 BP 553 EP 566 DI 10.5194/amt-8-553-2015 PG 14 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA CC7OR UT WOS:000350558300003 ER PT J AU Lundquist, JK Churchfield, MJ Lee, S Clifton, A AF Lundquist, J. K. Churchfield, M. J. Lee, S. Clifton, A. TI Quantifying error of lidar and sodar Doppler beam swinging measurements of wind turbine wakes using computational fluid dynamics SO ATMOSPHERIC MEASUREMENT TECHNIQUES LA English DT Article ID COMPLEX TERRAIN; TURBULENCE; FLOW AB Wind-profiling lidars are now regularly used in boundary-layer meteorology and in applications such as wind energy and air quality. Lidar wind profilers exploit the Doppler shift of laser light backscattered from particulates carried by the wind to measure a line-of-sight (LOS) velocity. The Doppler beam swinging (DBS) technique, used by many commercial systems, considers measurements of this LOS velocity in multiple radial directions in order to estimate horizontal and vertical winds. The method relies on the assumption of homogeneous flow across the region sampled by the beams. Using such a system in inhomogeneous flow, such as wind turbine wakes or complex terrain, will result in errors. To quantify the errors expected from such violation of the assumption of horizontal homogeneity, we simulate inhomogeneous flow in the atmospheric boundary layer, notably stably stratified flow past a wind turbine, with a mean wind speed of 6.5 m s(-1) at the turbine hub-height of 80 m. This slightly stable case results in 15 degrees of wind direction change across the turbine rotor disk. The resulting flow field is sampled in the same fashion that a lidar samples the atmosphere with the DBS approach, including the lidar range weighting function, enabling quantification of the error in the DBS observations. The observations from the instruments located upwind have small errors, which are ameliorated with time averaging. However, the downwind observations, particularly within the first two rotor diameters downwind from the wind turbine, suffer from errors due to the heterogeneity of the wind turbine wake. Errors in the stream-wise component of the flow approach 30% of the hub-height inflow wind speed close to the rotor disk. Errors in the cross-stream and vertical velocity components are also significant: cross-stream component errors are on the order of 15% of the hub-height inflow wind speed (1.0 m s(-1) /and errors in the vertical velocity measurement exceed the actual vertical velocity. By three rotor diameters downwind, DBS-based assessments of wake wind speed deficits based on the stream-wise velocity can be relied on even within the near wake within 1.0 m s(-1) (or 15% of the hub-height inflow wind speed), and the cross-stream velocity error is reduced to 8% while vertical velocity estimates are compromised. Measurements of inhomogeneous flow such as wind turbine wakes are susceptible to these errors, and interpretations of field observations should account for this uncertainty. C1 [Lundquist, J. K.] Univ Colorado, Dept Atmospher & Ocean Sci, Boulder, CO 80309 USA. [Lundquist, J. K.; Churchfield, M. J.; Lee, S.; Clifton, A.] Natl Renewable Energy Lab, Golden, CO USA. RP Lundquist, JK (reprint author), Univ Colorado, Dept Atmospher & Ocean Sci, Boulder, CO 80309 USA. EM julie.lundquist@colorado.edu OI Clifton, Andrew/0000-0001-9698-5083 FU US Department of Energy (DOE) [DE-AC36-08GO28308]; National Renewable Energy Laboratory; DOE Office of Energy Efficiency and Renewable Energy, Wind and Water Power Technologies Office; DOE's Office of Energy Efficiency and Renewable Energy FX This work was supported by the US Department of Energy (DOE) under Contract No. DE-AC36-08GO28308 with the National Renewable Energy Laboratory. The DOE Office of Energy Efficiency and Renewable Energy, Wind and Water Power Technologies Office provided funding for the work. The authors express appreciation to Branko Kosovic, three anonymous reviewers, and Valerie Kumer for helpful comments on the manuscript. The simulations were performed using computational resources sponsored by DOE's Office of Energy Efficiency and Renewable Energy and located at the National Renewable Energy Laboratory. NR 55 TC 13 Z9 13 U1 0 U2 14 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 2015 VL 8 IS 2 BP 907 EP 920 DI 10.5194/amt-8-907-2015 PG 14 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA CC7OR UT WOS:000350558300026 ER PT J AU Murphy, LJ Robertson, KN Kemp, RA Tuononen, HM Clyburne, JAC AF Murphy, Luke J. Robertson, Katherine N. Kemp, Richard A. Tuononen, Heikki M. Clyburne, Jason A. C. TI Structurally simple complexes of CO2 SO CHEMICAL COMMUNICATIONS LA English DT Article ID FRUSTRATED LEWIS PAIRS; CARBON-DIOXIDE COMPLEX; N-HETEROCYCLIC CARBENES; ANION PHOTOELECTRON-SPECTROSCOPY; METAL-ORGANIC FRAMEWORK; CRYSTAL-STRUCTURES; IONIC LIQUIDS; X-RAY; COORDINATION CHEMISTRY; GAS-PHASE AB The ability to bind CO2 through the formation of low-energy, easily-broken, bonds could prove invaluable in a variety of chemical contexts. For example, weak bonds to CO2 would greatly decrease the cost of the energy-intensive sorbent-regeneration step common to most carbon capture technologies. Furthermore, exploration of this field could lead to the discovery of novel CO2 chemistry. Reduction of complexed carbon dioxide might generate chemical feedstocks for the preparation of value-added products, particularly transportation fuels or fuel precursors. Implementation on a large scale could help to drastically reduce CO2 concentrations in the atmosphere. However, literature examples of weakly bonded complexes of CO2 are relatively few and true coordination complexes to a 'naked' CO2 fragment are nearly unheard of. In this review article, a variety of complexes of CO2 featuring diverse binding modes and reactivity will be examined. Topics covered include: (A) inclusion complexes of CO2 in porous materials. (B) Zwitterionic carbamates produced from the reaction of CO2 with polyamines. (C) Carbamate salts produced from reaction of CO2 with two equivalents of an amine. (D) Insertion products of CO2 into acid-base adducts (e.g., metal complexes). (E) Lewis acid-base activated CO2, such as frustrated Lewis pair complexes. (F) Simple base-CO2 adducts, wherein the base-CO2 bond is the only interaction formed. Complexes in the last category are of particular interest, and include imidazol-2-carboxylates (N-heterocyclic carbene adducts of CO2) as well as a few other examples that lie outside NHC chemistry. C1 [Murphy, Luke J.; Robertson, Katherine N.; Clyburne, Jason A. C.] St Marys Univ, Dept Chem, Atlantic Ctr Green Chem, Halifax, NS B3H 3C3, Canada. [Kemp, Richard A.] Univ New Mexico, Dept Chem, Albuquerque, NM 87131 USA. [Kemp, Richard A.] Sandia Natl Labs, Adv Mat Lab, Albuquerque, NM 87106 USA. [Tuononen, Heikki M.] Univ Jyvaskyla, Dept Chem, Ctr Neurosci, FI-40014 Jyvaskyla, Finland. RP Clyburne, JAC (reprint author), St Marys Univ, Dept Chem, Atlantic Ctr Green Chem, Halifax, NS B3H 3C3, Canada. EM jason.clyburne@smu.ca FU Natural Sciences and Engineering Research Council of Canada; Academy of Finland; Canada Research Chairs Program, Canadian Foundation for Innovation; Nova Scotia Research and Innovation Trust Fund; Foundation for Research of Natural Resources in Finland; University of Jyvaskyla; EnCana Corporation (Deep Panuke Education & Training and Research & Development Fund); National Science Foundation [CHE12-13529] FX We thank the Natural Sciences and Engineering Research Council of Canada (through the Discovery Grants Program to JACC) and the Academy of Finland (through its Research Fellowship to HMT). JACC acknowledges support from the Canada Research Chairs Program, the Canadian Foundation for Innovation and the Nova Scotia Research and Innovation Trust Fund. HMT acknowledges support from the Academy of Finland, the Foundation for Research of Natural Resources in Finland and the University of Jyvaskyla. This work was also supported, in part, by EnCana Corporation (Deep Panuke Education & Training and Research & Development Fund). RAK acknowledges support of the National Science Foundation (Grant CHE12-13529). NR 171 TC 31 Z9 31 U1 9 U2 149 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1359-7345 EI 1364-548X J9 CHEM COMMUN JI Chem. Commun. PY 2015 VL 51 IS 19 BP 3942 EP 3956 DI 10.1039/c4cc08510h PG 15 WC Chemistry, Multidisciplinary SC Chemistry GA CC2ZB UT WOS:000350212600001 PM 25601453 ER PT J AU Concepcion, JJ Zhong, DK Szalda, DJ Muckerman, JT Fujita, E AF Concepcion, Javier J. Zhong, Diane K. Szalda, David J. Muckerman, James T. Fujita, Etsuko TI Mechanism of water oxidation by [Ru(bda)(L)(2)]: the return of the "blue dimer" SO CHEMICAL COMMUNICATIONS LA English DT Article ID BRIDGED RUTHENIUM DIMER; ELECTRON-TRANSFER; PHOTOSYSTEM-II; SINGLE-SITE; CATALYST; COMPLEXES AB We describe here a combined solution-surface-DFT calculations study for complexes of the type [Ru(bda)(L)(2)] including X-ray structure of intermediates and their reactivity, as well as pH-dependent electro-chemistry and spectroelectrochemistry. These studies shed light on the mechanism of water oxidation by [Ru(bda)(L)(2)], revealing key features unavailable from solution studies with sacrificial oxidants. C1 [Concepcion, Javier J.; Zhong, Diane K.; Muckerman, James T.; Fujita, Etsuko] Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA. [Szalda, David J.] CUNY Bernard M Baruch Coll, Dept Nat Sci, New York, NY 10010 USA. RP Concepcion, JJ (reprint author), Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA. EM jconcepc@bnl.gov FU U.S. Department of Energy, Office of Science, Division of Chemical Sciences, Geosciences, & Biosciences, Office of Basic Energy Sciences [DE-AC02-98CH10886] FX This work was carried out at Brookhaven National Laboratory and supported by the U.S. Department of Energy, Office of Science, Division of Chemical Sciences, Geosciences, & Biosciences, Office of Basic Energy Sciences under contract DE-AC02-98CH10886. NR 22 TC 15 Z9 15 U1 7 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 2015 VL 51 IS 19 BP 4105 EP 4108 DI 10.1039/c4cc07968j PG 4 WC Chemistry, Multidisciplinary SC Chemistry GA CC2ZB UT WOS:000350212600037 PM 25670391 ER PT J AU Barrios, LA Salinas-Uber, J Roubeau, O Teat, SJ Aromi, G AF Barrios, L. A. Salinas-Uber, J. Roubeau, O. Teat, S. J. Aromi, G. TI Molecular self-recognition: a chiral [Mn(II)(6)] wheel via donor-acceptor pi center dot center dot center dot pi contacts and H-bonds SO CHEMICAL COMMUNICATIONS LA English DT Article ID SUPRAMOLECULAR CYLINDERS; COORDINATION CAGES; COMPLEXES; LIGAND; STATE; TRANSFORMATION; NAPHTHALENE; STACKING; NUCLEAR; METAL AB A multinucleating ligand capable of establishing different types of intermolecular interactions, when combined with acetate groups leads to the assembly of a chiral [Mn(II)(3)] cluster poised for a process of self-recognition through a combination of perfectly complementary weak forces. C1 [Barrios, L. A.; Salinas-Uber, J.; Aromi, G.] Univ Barcelona, Dept Quim Inorgan, E-08028 Barcelona, Spain. [Roubeau, O.] CSIC, Inst Ciencia Mat Aragon, E-50009 Zaragoza, Spain. [Roubeau, O.] Univ Zaragoza, E-50009 Zaragoza, Spain. [Teat, S. J.] Berkeley Lab, Adv Light Source, Berkeley, CA 94720 USA. RP Aromi, G (reprint author), Univ Barcelona, Dept Quim Inorgan, Diagonal 645, E-08028 Barcelona, Spain. RI Aromi, Guillem/I-2483-2015; Roubeau, Olivier/A-6839-2010; BARRIOS MORENO, LEONI ALEJANDRA/E-5413-2017 OI Aromi, Guillem/0000-0002-0997-9484; Roubeau, Olivier/0000-0003-2095-5843; BARRIOS MORENO, LEONI ALEJANDRA/0000-0001-7075-9950 FU ERC [258060 FuncMolQIP]; Spanish MICINN [MAT2011-24284]; Office of Science, Office of Basic Energy Sciences of the U.S. Department of Energy [DE-AC02-05CH11231] FX GA thanks the Generalitat de Catalunya for the prize ICREA Academia 2008 and 2013, for excellence in research and the ERC for a Starting Grant (258060 FuncMolQIP). The authors thank the Spanish MICINN for funding through MAT2011-24284 (OR), the ERC for a Predoctoral Fellowship (JSU) and a Postdoctoral contract (LAB) under Grant 258060 FuncMolQIP. 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 24 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 EI 1364-548X J9 CHEM COMMUN JI Chem. Commun. PY 2015 VL 51 IS 22 BP 4631 EP 4634 DI 10.1039/c5cc00142k PG 4 WC Chemistry, Multidisciplinary SC Chemistry GA CC6OX UT WOS:000350486300020 PM 25690703 ER PT J AU Liu, HD Xu, J Ma, CZ Meng, YS AF Liu, Haodong Xu, Jing Ma, Chuze Meng, Ying Shirley TI A new O3-type layered oxide cathode with high energy/power density for rechargeable Na batteries SO CHEMICAL COMMUNICATIONS LA English DT Article ID SODIUM-ION BATTERIES; X LESS-THAN; HIGH-CAPACITY CATHODE; POSITIVE ELECTRODE; LITHIUM BATTERIES; LI-BATTERIES; STABILITY; P2-TYPE; MN; NA4FE3(PO4)(2)(P2O7) AB A new O3-Na0.78Li0.18Ni0.25Mn0.583Ow is prepared as the cathode material for Na-ion batteries, delivering exceptionally high energy density and superior rate performance. The single-slope voltage profile and ex situ synchrotron X-ray diffraction data demonstrate that no phase transformation happens through a wide range of sodium concentrations (up to 0.8 Na removed). Ni2+/Ni4+ is suggested to be the main redox center. Further optimization could be realized by tuning the combination and the ratio of transition metals. C1 [Liu, Haodong; Xu, Jing; Ma, Chuze; Meng, Ying Shirley] Univ Calif San Diego, Dept NanoEngn, La Jolla, CA 92093 USA. [Xu, Jing] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. RP Meng, YS (reprint author), Univ Calif San Diego, Dept NanoEngn, 9500 Gilman Dr, La Jolla, CA 92093 USA. EM shirleymeng@ucsd.edu FU Northeastern Center for Chemical Energy Storage, an Energy Frontier Research Center - U.S. Department of Energy, Office of Basic Energy Sciences [DE-SC0012583]; China Scholarship Council [2011631005] FX Haodong Liu and Jing Xu equally contributed to this work. The authors are grateful for the financial support from the Northeastern Center for Chemical Energy Storage, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Basic Energy Sciences, with Award Number DE-SC0012583. H. Liu acknowledges the financial support from China Scholarship Council under Award Number 2011631005. The authors appreciate the kind assistance from Dr Baihua Qu for anode SnS2/rGO synthesis at National University of Singapore (NUS). The XAS and SXRD were collected on 20-BM-B and 11-BM respectively at Advanced Photon Source in Argonne National Laboratory. NR 44 TC 18 Z9 18 U1 8 U2 156 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1359-7345 EI 1364-548X J9 CHEM COMMUN JI Chem. Commun. PY 2015 VL 51 IS 22 BP 4693 EP 4696 DI 10.1039/c4cc09760b PG 4 WC Chemistry, Multidisciplinary SC Chemistry GA CC6OX UT WOS:000350486300036 PM 25692397 ER PT J AU Karan, NS Keller, AM Sampat, S Roslyak, O Arefin, A Hanson, CJ Casson, JL Desireddy, A Ghosh, Y Piryatinski, A Iyer, R Htoon, H Malko, AV Hollingsworth, JA AF Karan, Niladri S. Keller, Aaron M. Sampat, Siddharth Roslyak, Oleksiy Arefin, Ayesha Hanson, Christina J. Casson, Joanna L. Desireddy, Anil Ghosh, Yagnaseni Piryatinski, Andrei Iyer, Rashi Htoon, Han Malko, Anton V. Hollingsworth, Jennifer A. TI Plasmonic giant quantum dots: hybrid nanostructures for truly simultaneous optical imaging, photothermal effect and thermometry SO CHEMICAL SCIENCE LA English DT Article ID SUPPRESSED BLINKING; GOLD NANOPARTICLES; SHELL THICKNESS; NANOSHELLS; TEMPERATURE; GROWTH; PHOTOLUMINESCENCE; RESONANCES; MECHANISM; CANCER AB Hybrid semiconductor-metal nanoscale constructs are of both fundamental and practical interest. Semiconductor nanocrystals are active emitters of photons when stimulated optically, while the interaction of light with nanosized metal objects results in scattering and ohmic damping due to absorption. In a combined structure, the properties of both components can be realized together. At the same time, metal-semiconductor coupling may intervene to modify absorption and/or emission processes taking place in the semiconductor, resulting in a range of effects from photoluminescence quenching to enhancement. We show here that photostable 'giant' quantum dots when placed at the center of an ultrathin gold shell retain their key optical property of bright and blinking-free photoluminescence, while the metal shell imparts efficient photothermal transduction. The latter is despite the highly compact total particle size (40-60 nm "inorganic" diameter and <100 nm hydrodynamic diameter) and the very thin nature of the optically transparent Au shell. Importantly, the sensitivity of the quantum dot emission to local temperature provides a novel internal thermometer for recording temperature during infrared irradiation-induced photothermal heating. C1 [Karan, Niladri S.; Keller, Aaron M.; Hanson, Christina J.; Desireddy, Anil; Ghosh, Yagnaseni; Htoon, Han; Hollingsworth, Jennifer A.] Los Alamos Natl Lab, Ctr Integrated Nanotechnol, Mat Phys & Applicat Div, Los Alamos, NM 87545 USA. [Sampat, Siddharth; Malko, Anton V.] Univ Texas Dallas, Dept Phys, Richardson, TX 75080 USA. [Roslyak, Oleksiy] Fordham Univ, Dept Phys, Bronx, NY 10458 USA. [Arefin, Ayesha; Iyer, Rashi] Los Alamos Natl Lab, Def Syst & Anal Div, Syst Anal & Surveillance, Los Alamos, NM 87545 USA. [Casson, Joanna L.] Los Alamos Natl Lab, Div Chem, Phys Chem & Appl Spect, Los Alamos, NM 87545 USA. [Piryatinski, Andrei] Los Alamos Natl Lab, Div Theoret, Phys Condensed Matter & Complex Syst, Los Alamos, NM 87545 USA. RP Hollingsworth, JA (reprint author), Los Alamos Natl Lab, Ctr Integrated Nanotechnol, Mat Phys & Applicat Div, POB 1663, Los Alamos, NM 87545 USA. EM jenn@lanl.gov RI Piryatinski, Andrei/B-5543-2009; OI Htoon, Han/0000-0003-3696-2896 FU Division of Materials Science and Engineering (MSE), Office of Basic Energy Sciences (OBES), Office of Science (OS), U.S. Department of Energy (DOE) [2009LANL1096]; OBES, OS, DOE [DE-SC0010697]; Los Alamos National Laboratory (LANL) Directed Research and Development (LDRD) funds; LANL Center for Integrated Nanotechnologies (CINT) postdoctoral funding; OBES, OS, DOE MSE Biomolecular Materials Program; National Nuclear Security Administration of the U.S. Department of Energy [DE-AC52-06NA25396] FX For this effort, J.A.H., H.H., J.L.C and C.J.H. were supported by a Single Investigator Small Group Research Grant (2009LANL1096), Division of Materials Science and Engineering (MSE), Office of Basic Energy Sciences (OBES), Office of Science (OS), U.S. Department of Energy (DOE). A.V.M. and S.S were supported by grant DE-SC0010697, OBES, OS, DOE. N.S.K., A. A., Y.G. and R.I. were supported by Los Alamos National Laboratory (LANL) Directed Research and Development (LDRD) funds. A.M.K. and O.R. were supported by LANL Center for Integrated Nanotechnologies (CINT) postdoctoral funding. A.D. was supported by the OBES, OS, DOE MSE Biomolecular Materials Program. This work was performed in large part at CINT, a DOE, OBES Nanoscale Science Research Center and 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. We acknowledge the technical assistance from Piyush Bajaj in execution of the cell exposure experiments and analysis. We thank James Werner for instrumentation resources, helpful discussion regarding experimental design, and assistance in setting up the near-infrared irradiation with simultaneous photoluminescence imaging. NR 49 TC 10 Z9 10 U1 3 U2 42 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2041-6520 EI 2041-6539 J9 CHEM SCI JI Chem. Sci. PY 2015 VL 6 IS 4 BP 2224 EP 2236 DI 10.1039/c5sc00020c PG 13 WC Chemistry, Multidisciplinary SC Chemistry GA CD9IW UT WOS:000351412800012 ER PT J AU Katz, MJ Moon, SY Mondloch, JE Beyzavi, MH Stephenson, CJ Hupp, JT Farha, OK AF Katz, Michael J. Moon, Su-Young Mondloch, Joseph E. Beyzavi, M. Hassan Stephenson, Casey J. Hupp, Joseph T. Farha, Omar K. TI Exploiting parameter space in MOFs: a 20-fold enhancement of phosphate-ester hydrolysis with UiO-66-NH2 SO CHEMICAL SCIENCE LA English DT Article ID METAL-ORGANIC FRAMEWORKS; BIMETALLIC TETRABENZIMIDAZOLE COMPLEXES; BACTERIAL PHOSPHOTRIESTERASE; CATALYTIC DECOMPOSITION; REACTION-MECHANISM; ARYL PHOSPHATE; METHANOLYSIS; DEGRADATION; PHOSPHORUS; STABILITY AB The hydrolysis of nerve agents is of primary concern due to the severe toxicity of these agents. Using a MOF-based catalyst (UiO-66), we have previously demonstrated that the hydrolysis can occur with relatively fast half-lives of 50 minutes. However, these rates are still prohibitively slow to be efficiently utilized for some practical applications (e.g., decontamination wipes used to clean exposed clothing/skin/vehicles). We thus turned our attention to derivatives of UiO-66 in order to probe the importance of functional groups on the hydrolysis rate. Three UiO-66 derivatives were explored; UiO-66-NO2 and UiO-66-(OH)(2) showed little to no change in hydrolysis rate. However, UiO-66-NH2 showed a 20 fold increase in hydrolysis rate over the parent UiO-66 MOF. Half-lives of 1 minute were observed with this MOF. In order to probe the role of the amino moiety, we turned our attention to UiO-67, UiO-67-NMe2 and UiO-67-NH2. In these MOFs, the amino moiety is in close proximity to the zirconium node. We observed that UiO-67-NH2 is a faster catalyst than UiO-67 and UiO-67-NMe2. We conclude that the role of the amino moiety is to act as a proton-transfer agent during the catalytic cycle and not to hydrogen bond or to form a phosphorane intermediate. C1 [Katz, Michael J.; Moon, Su-Young; Mondloch, Joseph E.; Beyzavi, M. Hassan; Stephenson, Casey J.; Hupp, Joseph T.; Farha, Omar K.] Northwestern Univ, Dept Chem, Evanston, IL 60208 USA. [Hupp, Joseph T.] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. [Farha, Omar K.] King Abdulaziz Univ, Fac Sci, Dept Chem, Jeddah 21413, Saudi Arabia. RP Hupp, JT (reprint author), Northwestern Univ, Dept Chem, 2145 Sheridan Rd, Evanston, IL 60208 USA. EM j-hupp@northwestern.edu; o-farha@northwestern.edu RI Faculty of, Sciences, KAU/E-7305-2017; OI Katz, Michael/0000-0002-7744-3956 FU DTRA [HDTRA-1-10-0023] FX O.K.F. and J.T.H. gratefully acknowledges DTRA for financial support (grant HDTRA-1-10-0023). The authors would like to thank Nicolaas Vermeulen for his assistance in the purification of methy-paraoxon. NR 71 TC 34 Z9 35 U1 41 U2 169 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2041-6520 EI 2041-6539 J9 CHEM SCI JI Chem. Sci. PY 2015 VL 6 IS 4 BP 2286 EP 2291 DI 10.1039/c4sc03613a PG 6 WC Chemistry, Multidisciplinary SC Chemistry GA CD9IW UT WOS:000351412800017 ER PT J AU Kwant, RL Jaffe, J Palmere, PJ Francis, MB AF Kwant, Richard L. Jaffe, Jake Palmere, Peter J. Francis, Matthew B. TI Controlled levels of protein modification through a chromatography-mediated bioconjugation SO CHEMICAL SCIENCE LA English DT Article ID ANTIBODY DRUG CONJUGATE; AFFINITY-CHROMATOGRAPHY; LIVING CELLS; AMINOPHENOLS; SYSTEM; IDENTIFICATION; PURIFICATION; ANILINES; AGAROSE; DNA AB Synthetically modified proteins are increasingly finding applications as well-defined scaffolds for materials. In practice it remains difficult to construct bioconjugates with precise levels of modification because of the limited number of repeated functional groups on proteins. This article describes a method to control the level of protein modification in cases where there exist multiple potential modification sites. A protein is first tagged with a handle using any of a variety of modification chemistries. This handle is used to isolate proteins with a particular number of modifications via affinity chromatography, and then the handle is elaborated with a desired moiety using an oxidative coupling reaction. This method results in a sample of protein with a well-defined number of modifications, and we find it particularly applicable to systems like protein homomultimers in which there is no way to discern between chemically identical subunits. We demonstrate the use of this method in the construction of a protein-templated light-harvesting mimic, a type of system which has historically been difficult to make in a well-defined manner. C1 [Kwant, Richard L.; Jaffe, Jake; Palmere, Peter J.; Francis, Matthew B.] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. [Francis, Matthew B.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. RP Francis, MB (reprint author), Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. EM mbfrancis@berkeley.edu FU Office of Science, Chemical Sciences, Geosciences, and Biosciences Division, of the U.S. Department of Energy [DEAC02-05CH11231]; Department of Defense (DoD) through the National Defense Science & Engineering Graduate Fellowship (NDSEG) Program FX The development of the beta-cyclodextrin-based chromatography technique was supported by the Energy Biosciences Institute at UC Berkeley. Our studies of protein-templated light harvesting systems were generously supported by the Director, Office of Science, Chemical Sciences, Geosciences, and Biosciences Division, of the U.S. Department of Energy under Contract no. DEAC02-05CH11231. R.L.K. was supported by the Department of Defense (DoD) through the National Defense Science & Engineering Graduate Fellowship (NDSEG) Program. NR 29 TC 1 Z9 1 U1 1 U2 18 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2041-6520 EI 2041-6539 J9 CHEM SCI JI Chem. Sci. PY 2015 VL 6 IS 4 BP 2596 EP 2601 DI 10.1039/c4sc03790a PG 6 WC Chemistry, Multidisciplinary SC Chemistry GA CD9IW UT WOS:000351412800057 ER PT J AU Luthi, MP Ryser, C Andrews, LC Catania, GA Funk, M Hawley, RL Hoffman, MJ Neumann, TA AF Luethi, M. P. Ryser, C. Andrews, L. C. Catania, G. A. Funk, M. Hawley, R. L. Hoffman, M. J. Neumann, T. A. TI Heat sources within the Greenland Ice Sheet: dissipation, temperate paleo-firn and cryo-hydrologic warming SO CRYOSPHERE LA English DT Article ID ABLATION ZONE; WEST GREENLAND; FAST-FLOW; JAKOBSHAVNS-ISBRAE; DARK REGION; MECHANISMS; DEFORMATION; BOREHOLES; MOTION; LEVEL AB Ice temperature profiles from the Greenland Ice Sheet contain information on the deformation history, past climates and recent warming. We present full-depth temperature profiles from two drill sites on a flow line passing through Swiss Camp, West Greenland. Numerical modeling reveals that ice temperatures are considerably higher than would be expected from heat diffusion and dissipation alone. The possible causes for this extra heat are evaluated using a Lagrangian heat flow model. The model results reveal that the observations can be explained with a combination of different processes: enhanced dissipation (strain heating) in ice-age ice, temperate paleo-firn, and cryo-hydrologic warming in deep crevasses. C1 [Luethi, M. P.; Ryser, C.; Funk, M.] ETH, Versuchsanstalt Wasserbau Hydrol & Glaziol VAW, CH-8093 Zurich, Switzerland. [Andrews, L. C.; Catania, G. A.] Univ Texas Austin, Inst Geophys, Austin, TX 78758 USA. [Andrews, L. C.; Catania, G. A.] Univ Texas Austin, Dept Geol Sci, Austin, TX 78758 USA. [Hawley, R. L.] Dartmouth Coll, Dept Earth Sci, Hanover, NH 03755 USA. [Hoffman, M. J.] Los Alamos Natl Lab, Fluid Dynam & Solid Mech Grp, Los Alamos, NM 87545 USA. [Neumann, T. A.] NASA, Goddard Space Flight Ctr, Greenbelt, MD 20770 USA. RP Luthi, MP (reprint author), ETH, Versuchsanstalt Wasserbau Hydrol & Glaziol VAW, CH-8093 Zurich, Switzerland. EM martin.luethi@geo.uzh.ch RI Catania, Ginny/B-9787-2008; Neumann, Thomas/D-5264-2012; Andrews, Lauren/D-8274-2017; OI Andrews, Lauren/0000-0003-3727-4737; Luthi, Martin Peter/0000-0003-4419-8496 FU Swiss National Science Foundation [200021_127197]; US-NSF [OPP 0908156, OPP 0909454, ANT-0424589]; NASA within the US Department of Energy Office of Science FX This project was supported by Swiss National Science Foundation Grant 200021_127197, US-NSF Grants OPP 0908156, OPP 0909454 and ANT-0424589 (to CReSIS), NASA Cryospheric Sciences, and Climate Modeling Programs within the US Department of Energy Office of Science. Logistical support was provided by CH2MHill Polar Services. NR 37 TC 10 Z9 10 U1 4 U2 5 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1994-0416 EI 1994-0424 J9 CRYOSPHERE JI Cryosphere PY 2015 VL 9 IS 1 BP 245 EP 253 DI 10.5194/tc-9-245-2015 PG 9 WC Geography, Physical; Geosciences, Multidisciplinary SC Physical Geography; Geology GA CC7NR UT WOS:000350555400018 ER PT J AU Mittal, A Vinzant, TB Brunecky, R Black, SK Pilath, HM Himmel, ME Johnson, DK AF Mittal, Ashutosh Vinzant, Todd B. Brunecky, Roman Black, Stuart K. Pilath, Heidi M. Himmel, Michael E. Johnson, David K. TI Investigation of the role of lignin in biphasic xylan hydrolysis during dilute acid and organosolv pretreatment of corn stover SO GREEN CHEMISTRY LA English DT Article ID MAIZE CELL-WALLS; ENZYMATIC-HYDROLYSIS; HEMICELLULOSE HYDROLYSIS; LIGNOCELLULOSIC BIOMASS; REACTION-KINETICS; SUGAR MAPLE; WOOD; AUTOHYDROLYSIS; CELLULOSE; ETHANOL AB One of the key objectives of biomass pretreatment is to maximize the xylose yield. However, the kinetics of xylan hydrolysis appear to be governed by two parallel first-order reactions with one reaction much faster than the other, thereby limiting both the rate and extent of xylan hydrolysis. Here, we investigate the influence of lignin on xylan hydrolysis kinetics during dilute acid pretreatment of corn stover rind (CSR) by modifying either the substrate or the pretreatment conditions. Dilute acid pretreatment was conducted to test the hypothesis that association of a fraction of the xylan with lignin causes this fraction to hydrolyze at a slower rate resulting in biphasic kinetics. In addition, CSR was pretreated under organosolv (OS) conditions, where xylan and lignin were solubilized simultaneously, to decouple the hydrolysis of xylan from the lignin redistribution process that occurs during dilute acid pretreatment. Dilute acid pretreatment of CSR delignified under mild conditions still exhibited biphasic kinetics, although the fraction of slow hydrolyzing xylan decreased and the rate of fast hydrolyzing xylan increased by 60% resulting in achieving more than 95% total xylose yield. Pretreatment of CSR under OS conditions also appeared to exhibit biphasic xylan hydrolysis kinetics. Unexpectedly, the solubilization of xylan and lignin appeared to occur at similar rates. The increases in the rate and fraction of fast hydrolyzing xylan observed by removing the majority of the lignin support the hypothesis that the slow hydrolyzing xylan is a result of its association with lignin. To further investigate the role of lignin in xylan hydrolysis, the raw and pretreated CSR samples were labeled with a monoclonal antibody (containing a fluorescent dye) that binds xylan specifically so that the location of xylan in the cell wall could be imaged by confocal laser scanning microscopy (CLM). CLM of the pretreated delignified samples showed a similar, intense signal pattern as exhibited by the raw and pretreated control, indicating that the majority of the remaining xylan was located at both cytosolic and middle lamellar cell wall edges. OS pretreated CSR did, however, show a diminution in signal intensity at cell wall edges compared to CSR pretreated under standard dilute acid conditions. C1 [Mittal, Ashutosh; Vinzant, Todd B.; Brunecky, Roman; Himmel, Michael E.; Johnson, David K.] Natl Renewable Energy Lab, Biosci Ctr, Golden, CO 80401 USA. [Black, Stuart K.; Pilath, Heidi M.] Natl Renewable Energy Lab, Natl Bioenergy Ctr, Golden, CO 80401 USA. RP Mittal, A (reprint author), Natl Renewable Energy Lab, Biosci Ctr, 15013 Denver W Pkwy, Golden, CO 80401 USA. EM ashutosh.mittal@nrel.gov FU U.S. Department of Energy (DOE) [DE-AC36-08GO28308]; DOE Office of Energy Efficiency and Renewable Energy, Bioenergy Technologies Office (BETO) FX This work was supported by the U.S. Department of Energy (DOE) under Contract No. DE-AC36-08GO28308. Funding for the work was provided by the DOE Office of Energy Efficiency and Renewable Energy, Bioenergy Technologies Office (BETO). NR 43 TC 3 Z9 3 U1 8 U2 33 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9262 EI 1463-9270 J9 GREEN CHEM JI Green Chem. PY 2015 VL 17 IS 3 BP 1546 EP 1558 DI 10.1039/c4gc02258k PG 13 WC Chemistry, Multidisciplinary; GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY SC Chemistry; Science & Technology - Other Topics GA CD4YC UT WOS:000351091300025 ER PT J AU George, A Brandt, A Tran, K Zahari, SMSNS Klein-Marcuschamer, D Sun, N Sathitsuksanoh, N Shi, J Stavila, V Parthasarathi, R Singh, S Holmes, BM Welton, T Simmons, BA Hallett, JP AF George, Anthe Brandt, Agnieszka Tran, Kim Zahari, Shahrul M. S. Nizan S. Klein-Marcuschamer, Daniel Sun, Ning Sathitsuksanoh, Noppadon Shi, Jian Stavila, Vitalie Parthasarathi, Ramakrishnan Singh, Seema Holmes, Bradley M. Welton, Tom Simmons, Blake A. Hallett, Jason P. TI Design of low-cost ionic liquids for lignocellulosic biomass pretreatment SO GREEN CHEMISTRY LA English DT Article ID PSEUDO-LIGNIN; CORN STOVER; DILUTE-ACID; DECONSTRUCTION; SWITCHGRASS; AFEX(TM) AB The cost of ionic liquids (ILs) is one of the main impediments to IL utilization in the cellulosic biorefinery, especially in the pretreatment step. In this study, a number of ionic liquids were synthesized with the goal of optimizing solvent cost and stability whilst demonstrating promising processing potential. To achieve this, inexpensive feedstocks such as sulfuric acid and simple amines were combined into a range of protic ionic liquids containing the hydrogen sulfate [HSO4](-) anion. The performance of these ionic liquids was compared to a benchmark system containing the IL 1-ethyl-3-methylimidazolium acetate [C(2)C(1)im][OAc]. The highest saccharification yields were observed for the triethylammonium hydrogen sulfate IL, which was 75% as effective as the benchmark system. Techno-economic modeling revealed that this promising and yet to be optimized yield was achieved at a fraction of the processing cost. This study demonstrates that some ILs can compete with the cheapest pretreatment chemicals, such as ammonia, in terms of effectiveness and process cost, removing IL cost as a barrier to the economic viability of IL-based biorefineries. C1 [George, Anthe; Tran, Kim; Klein-Marcuschamer, Daniel; Sun, Ning; Sathitsuksanoh, Noppadon; Shi, Jian; Stavila, Vitalie; Parthasarathi, Ramakrishnan; Singh, Seema; Holmes, Bradley M.; Simmons, Blake A.] Joint BioEnergy Inst, Emeryville, CA 94608 USA. [Brandt, Agnieszka; Zahari, Shahrul M. S. Nizan S.; Hallett, Jason P.] Univ London Imperial Coll Sci Technol & Med, Dept Chem Engn, London SW7 2AZ, England. [Zahari, Shahrul M. S. Nizan S.; Welton, Tom] Univ London Imperial Coll Sci Technol & Med, Dept Chem, London SW7 2AY, England. RP George, A (reprint author), Joint BioEnergy Inst, Emeryville, CA 94608 USA. EM j.hallett@imperial.ac.uk RI Hallett, Jason/A-3281-2012; Brandt, Agnieszka/H-5966-2011; OI Hallett, Jason/0000-0003-3431-2371; Brandt, Agnieszka/0000-0002-5805-0233; Simmons, Blake/0000-0002-1332-1810 FU Office of Science, Office of Biological and Environmental Research, of the U.S. Department of Energy [DE-AC02-05CH11231] FX This work conducted by the Joint BioEnergy Institute was supported by the Office of Science, Office of Biological and Environmental Research, of the U.S. Department of Energy under Contract no. DE-AC02-05CH11231. NR 29 TC 49 Z9 50 U1 22 U2 109 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1463-9262 EI 1463-9270 J9 GREEN CHEM JI Green Chem. PY 2015 VL 17 IS 3 BP 1728 EP 1734 DI 10.1039/c4gc01208a PG 7 WC Chemistry, Multidisciplinary; GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY SC Chemistry; Science & Technology - Other Topics GA CD4YC UT WOS:000351091300046 ER PT J AU Stephenson, KE Neubauer, GH Reimer, U Pawlowski, N Knaute, T Zervveck, J Korber, BT Barouch, DH AF Stephenson, Kathryn E. Neubauer, George H. Reimer, Ulf Pawlowski, Nikolaus Knaute, Tobias Zervveck, Johannes Korber, Bette T. Barouch, Dan H. TI Quantification of the epitope diversity of HIV-1-specific binding antibodies by peptide microarrays for global HIV-1 vaccine development SO JOURNAL OF IMMUNOLOGICAL METHODS LA English DT Article DE HIV; Peptide microarray; Diversity; Antibody; Vaccine ID HUMAN-IMMUNODEFICIENCY-VIRUS; B-CELL RESPONSES; RHESUS-MONKEYS; IGG ANTIBODIES; INFECTION; BREADTH; CHALLENGES; SIGNATURES; EFFICACY; IMMUNITY AB An effective vaccine against human immunodeficiency virus type 1 (HIV-1) will have to provide protection against a vast array of different HIV-1 strains. Current methods to measure HIV-1-specific binding antibodies following immunization typically focus on determining the magnitude of antibody responses, but the epitope diversity of antibody responses has remained largely unexplored. Here we describe the development of a global HIV-1 peptide microarray that contains 6564 peptides from across the HIV-1 proteome and covers the majority of HIV-1 sequences in the Los Alamos National Laboratory global HIV-1 sequence database. Using this microarray, we quantified the magnitude, breadth, and depth of IgG binding to linear HIV-1 sequences in HIV-1-infected humans and HIV-1-vaccinated humans, rhesus monkeys and guinea pigs. The microarray measured potentially important differences in antibody epitope diversity, particularly regarding the depth of epitope variants recognized at each binding site. Our data suggest that the global HIV-1 peptide microarray may be a useful tool for both preclinical and clinical HIV-1 research. (C) 2014 The Authors. Published by Elsevier B.V. C1 [Stephenson, Kathryn E.; Neubauer, George H.; Barouch, Dan H.] Beth Israel Deaconess Med Ctr, Ctr Virol & Vaccine Res, Boston, MA 02215 USA. [Reimer, Ulf; Pawlowski, Nikolaus; Knaute, Tobias; Zervveck, Johannes] JPT Peptide Technol, Berlin, Germany. [Korber, Bette T.] Los Alamos Natl Lab, Div Theoret, Los Alamos, NM USA. [Barouch, Dan H.] Ragon Inst MGH MIT & Harvard, Boston, MA USA. RP Barouch, DH (reprint author), Beth Israel Deaconess Med Ctr, Ctr Virol & Vaccine Res, 330 Brookline Ave,E CLS-1047, Boston, MA 02215 USA. EM dbarouch@bidmc.harvard.edu FU National Institutes of Health [AI060354, AI078526, AI084794, AI095985, AI096040]; Bill and Melinda Gates Foundation [OPP 1033091, OPP1040741]; Ragon Institute of MGH, MIT, and Harvard FX This research was supported by the National Institutes of Health (AI060354 to K.E.S.; AI078526, AI084794, AI095985, and AI096040 to D.H.B.), the Bill and Melinda Gates Foundation (OPP 1033091, OPP1040741 to D.H.B.), and the Ragon Institute of MGH, MIT, and Harvard (to K.E.S. and D.H.B.). Plasma and serum samples from human subjects were obtained from studies conducted by the AIDS Clinical Trials Group and the NIH Integrated Preclinical/Clinical AIDS Vaccine Development Program. We thank E. Rosenberg, L Baden, M. Seaman, C. Bricault, J. Iampietro, H. Li, and Z. Kang for providing generous advice, assistance, and reagents. NR 41 TC 6 Z9 6 U1 0 U2 3 PU ELSEVIER SCIENCE BV PI AMSTERDAM PA PO BOX 211, 1000 AE AMSTERDAM, NETHERLANDS SN 0022-1759 EI 1872-7905 J9 J IMMUNOL METHODS JI J. Immunol. Methods PD JAN PY 2015 VL 416 BP 105 EP 123 DI 10.1016/j.jim.2014.11.006 PG 19 WC Biochemical Research Methods; Immunology SC Biochemistry & Molecular Biology; Immunology GA CC9UC UT WOS:000350715700010 PM 25445329 ER PT J AU Wu, Y Ma, C Yang, JH Li, ZC Allard, LF Liang, CD Chi, MF AF Wu, Yan Ma, Cheng Yang, Jihui Li, Zicheng Allard, Lawrence F. Liang, Chengdu Chi, Miaofang TI Probing the initiation of voltage decay in Li-rich layered cathode materials at the atomic scale SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID LITHIUM-ION BATTERIES; SPINEL COMPOSITE CATHODES; X-RAY-DIFFRACTION; ELECTRON-MICROSCOPY; CAPACITY; OXIDES; ELECTROCHEMISTRY; CHALLENGES; DESIGN; NI AB Li-rich layered oxides hold great promise for improving the energy density of present-day Li-ion batteries. Their application is, however, limited by the voltage decay upon cycling, and the origin of such a phenomenon is poorly understood. A major issue is determining the voltage range over which detrimental reactions originate. In the present study, a unique yet effective approach was employed to probe this issue. Instead of studying the materials during the first cycle, electrochemical behavior and evolution of the atomic structures were compared in extensively cycled specimens under varied charge/discharge voltages. With the upper cutoff voltage lowered from 4.8 to 4.4 V, the voltage decay ceased to occur even after 60 cycles. In the meantime, the material maintained its layered structure without any spinel phase emerging at the surface, which is unambiguously shown by the atomic-resolution Z-contrast imaging and electron energy loss spectroscopy. These results have conclusively demonstrated that structural/chemical changes responsible for the voltage decay began between 4.4 and 4.8 V, where the layered-to-spinel transition was the most dramatic structural change observed. This discovery lays important groundwork for the mechanistic understanding of the voltage decay in Li-rich layered cathode materials. C1 [Wu, Yan] Gen Motors Global R&D Ctr, Warren, MI 48090 USA. [Ma, Cheng; Allard, Lawrence F.; Liang, Chengdu; Chi, Miaofang] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. [Yang, Jihui] Univ Washington, Dept Mat Sci & Engn, Seattle, WA 98195 USA. [Li, Zicheng] Optimal Inc, Plymouth, MI 48170 USA. RP Wu, Y (reprint author), Gen Motors Global R&D Ctr, 30500 Mound Rd, Warren, MI 48090 USA. EM yan.wu@gm.com; jihuiy@uw.edu; chim@ornl.gov RI Yang, Jihui/A-3109-2009; Ma, Cheng/C-9120-2014; Chi, Miaofang/Q-2489-2015 OI Chi, Miaofang/0000-0003-0764-1567 FU U.S. Department of Energy, Office of Science, Materials Sciences and Engineering Division FX The microscopic work was performed as in-house research at the Center for Nanophase Materials Sciences (CNMS), which is an Office of Science User Facility. Work on the electrochemical analysis at ORNL was supported by the U.S. Department of Energy, Office of Science, Materials Sciences and Engineering Division, and performed at the CNMS. J. Yang would like to thank the support from the Inamori Foundation. NR 27 TC 14 Z9 14 U1 7 U2 101 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7488 EI 2050-7496 J9 J MATER CHEM A JI J. Mater. Chem. A PY 2015 VL 3 IS 10 BP 5385 EP 5391 DI 10.1039/c4ta06856d PG 7 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA CC9IJ UT WOS:000350682100021 ER PT J AU Liao, C Sa, N Key, B Burrell, AK Cheng, L Curtiss, LA Vaughey, JT Woo, JJ Hu, LB Pan, BF Zhang, ZC AF Liao, Chen Sa, Niya Key, Baris Burrell, Anthony K. Cheng, Lei Curtiss, Larry A. Vaughey, John T. Woo, Jung-Je Hu, Libo Pan, Baofei Zhang, Zhengcheng TI The unexpected discovery of the Mg(HMDS)(2)/MgCl2 complex as a magnesium electrolyte for rechargeable magnesium batteries SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID ENERGY-STORAGE; DEPOSITION; CHALLENGE; CATHODE; SALTS AB We developed a unique class of non-Grignard, aluminum-free magnesium electrolytes based on a simple mixture of magnesium compounds: magnesium hexamethyldisilazide (Mg(HMDS)(2)) and magnesium chloride (MgCl2). Through a reverse Schlenk equilibrium, a concentrated THF solution of Mg(HMDS)(2)-4MgCl(2) was prepared to achieve reversible Mg deposition/dissolution, a wide electrochemical window, and a coulombic efficiency of 99%. High reversible capacities and good rate capabilities were obtained in Mg-Mo6S8 cells using these new electrolytes in tests with different rates. The unexpected high solubility of MgCl2 in the solvent of THF with the help from Mg(HMDS)(2) provides a new way to develop magnesium electrolytes. C1 [Liao, Chen; Sa, Niya; Key, Baris; Burrell, Anthony K.; Vaughey, John T.; Pan, Baofei] Argonne Natl Lab, Joint Ctr Energy Storage Res, Lemont, IL 60439 USA. [Liao, Chen; Sa, Niya; Key, Baris; Burrell, Anthony K.; Vaughey, John T.; Woo, Jung-Je; Hu, Libo; Pan, Baofei; Zhang, Zhengcheng] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. [Cheng, Lei; Curtiss, Larry A.] Argonne Natl Lab, Mat Sci Div, Argonne, IL 60439 USA. RP Liao, C (reprint author), Argonne Natl Lab, Joint Ctr Energy Storage Res, Lemont, IL 60439 USA. EM liaoc@anl.gov RI Pan, Baofei/H-2867-2015; SA, NIYA/E-8521-2017; OI Liao, Chen/0000-0001-5168-6493 FU Joint Center for Energy Storage Research, an Energy Innovation Hub - U.S. Department of Energy, Office of Science, Basic Energy Sciences; U.S. Department of Energy Office of Science laboratory [DE-AC02-06CH11357] FX This work was supported as part of the Joint Center for Energy Storage Research, an Energy Innovation Hub funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences. 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 electron microscopy was accomplished at the Electron Microscopy Center at Argonne National Laboratory. NR 19 TC 18 Z9 18 U1 15 U2 78 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7488 EI 2050-7496 J9 J MATER CHEM A JI J. Mater. Chem. A PY 2015 VL 3 IS 11 BP 6082 EP 6087 DI 10.1039/c5ta00118h PG 6 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA CD2EH UT WOS:000350886600039 ER PT J AU Zou, JD Paudyal, D Liu, J Mudryk, Y Pecharsky, VK Gschneidner, KA AF Zou, Junding Paudyal, Durga Liu, Jing Mudryk, Yaroslav Pecharsky, Vitalij K. Gschneidner, Karl A., Jr. TI Magnetostructural phase transformations in Tb1-xMn2 SO JOURNAL OF MATERIALS CHEMISTRY C LA English DT Article ID TBMN2 INTERMETALLIC COMPOUND; MN-MOMENT INSTABILITY; RARE-EARTH; MAGNETIC-PROPERTIES; RMN2 COMPOUNDS; LAVES PHASES; X-RAY; TRANSITION; FIELD; YMN2 AB Magnetism and phase transformations in non-stoichiometric Tb1-xMn2 (x = 0.056, 0.039) have been studied as functions of temperature and magnetic field using magnetization, heat capacity, and X-ray powder diffraction measurements. Upon lowering the temperature, the compounds sequentially order ferrimagnetically and antiferromagnetically, and finally, exhibit spin reorientation transitions. Structural distortions from room temperature cubic to low temperature rhombohedral structures occur at T-N, and are accompanied by large volume changes reaching similar to-1.27% and -1.42%, respectively. First principles electronic structure calculations confirm the phase transformation from the ferrimagnetic cubic structure to the antiferromagnetic rhombohedral structure in TbMn2. C1 [Zou, Junding] Zhejiang Univ, Sch Mat Sci & Engn, State Key Lab Silicon Mat, Key Lab Novel Mat Informat Technol Zhejiang Prov, Hangzhou 310027, Zhejiang, Peoples R China. [Zou, Junding; Paudyal, Durga; Liu, Jing; Mudryk, Yaroslav; Pecharsky, Vitalij K.; Gschneidner, Karl A., Jr.] Iowa State Univ, US Dept Energy, Ames Lab, Ames, IA 50011 USA. [Liu, Jing; Pecharsky, Vitalij K.; Gschneidner, Karl A., Jr.] Iowa State Univ, Dept Mat Sci & Engn, Ames, IA 50011 USA. RP Zou, JD (reprint author), Zhejiang Univ, Sch Mat Sci & Engn, State Key Lab Silicon Mat, Key Lab Novel Mat Informat Technol Zhejiang Prov, Hangzhou 310027, Zhejiang, Peoples R China. EM zoujd@zju.edu.cn FU National Natural Science Foundation of China [51471150]; U.S. Department of Energy, Office of Basic Energy Science, Division of Materials Sciences and Engineering; U.S. Department of Energy by Iowa State University [DE-AC02-07CH11358] FX This work was supported by the National Natural Science Foundation of China (Grant no. 51471150). Work at the Ames Laboratory was supported by the U.S. Department of Energy, Office of Basic Energy Science, Division of Materials Sciences and Engineering. The research was performed at the Ames Laboratory operated for the U.S. Department of Energy by Iowa State University under Contract no. DE-AC02-07CH11358. NR 45 TC 1 Z9 1 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 EI 2050-7534 J9 J MATER CHEM C JI J. Mater. Chem. C PY 2015 VL 3 IS 10 BP 2422 EP 2430 DI 10.1039/c4tc02506g PG 9 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA CC9LY UT WOS:000350693200032 ER PT J AU Dhak, D Hong, S Das, S Dhak, P AF Dhak, Debasis Hong, Seungbum Das, Soma Dhak, Prasanta TI Synthesis, Characterization, Properties, and Applications of Nanosized Ferroelectric, Ferromagnetic, or Multiferroic Materials SO JOURNAL OF NANOMATERIALS LA English DT Editorial Material C1 [Dhak, Debasis] Sidho Kanho Birsha Univ, Dept Chem, Purulia 723101, W Bengal, India. [Hong, Seungbum] Argonne Natl Lab, Div Mat Sci, Lemont, IL 60439 USA. [Das, Soma] Guru Ghasidas Vishwavidyalaya, Inst Technol, Elect & Commun Engn, Bilaspur 495009, India. [Dhak, Prasanta] Seoul Natl Univ, Dept Mat Sci & Engn, Seoul 151744, South Korea. RP Dhak, D (reprint author), Sidho Kanho Birsha Univ, Dept Chem, Purulia 723101, W Bengal, India. EM debasisdhak@yahoo.co.in RI Hong, Seungbum/B-7708-2009 OI Hong, Seungbum/0000-0002-2667-1983 FU US Department of Energy, Office of Science, Materials Sciences and Engineering Division FX We would like to thank our reviewers for their time and comments and thank the authors for their contributions to this special issue. This special issue could not have been successful without their contribution and support. The work at Argonne (Seungbum Hong was responsible for paper writing) was supported by the US Department of Energy, Office of Science, Materials Sciences and Engineering Division. NR 0 TC 0 Z9 0 U1 0 U2 5 PU HINDAWI PUBLISHING CORPORATION PI NEW YORK PA 410 PARK AVENUE, 15TH FLOOR, #287 PMB, NEW YORK, NY 10022 USA SN 1687-4110 EI 1687-4129 J9 J NANOMATER JI J. Nanomater. PY 2015 AR 723145 DI 10.1155/2015/723145 PG 2 WC Nanoscience & Nanotechnology; Materials Science, Multidisciplinary SC Science & Technology - Other Topics; Materials Science GA CD5FN UT WOS:000351113400001 ER PT J AU Diefenderfer, HL AF Diefenderfer, Heida L. TI Coastal Conservation SO MARINE BIOLOGY RESEARCH LA English DT Book Review C1 [Diefenderfer, Heida L.] Pacific NW Natl Lab, Coastal Sci Div, Marine Sci Lab, Sequim, WA 98382 USA. RP Diefenderfer, HL (reprint author), Pacific NW Natl Lab, Coastal Sci Div, Marine Sci Lab, Sequim, WA 98382 USA. EM heida.diefenderfer@pnnl.gov NR 6 TC 0 Z9 0 U1 1 U2 1 PU TAYLOR & FRANCIS AS PI OSLO PA KARL JOHANS GATE 5, NO-0154 OSLO, NORWAY SN 1745-1000 EI 1745-1019 J9 MAR BIOL RES JI Mar. Biol. Res. PY 2015 VL 11 IS 4 BP 446 EP 448 DI 10.1080/17451000.2014.999095 PG 3 WC Ecology; Marine & Freshwater Biology SC Environmental Sciences & Ecology; Marine & Freshwater Biology GA CD3MO UT WOS:000350983000014 ER PT J AU Rus, SF Herklotz, A AF Rus, S. F. Herklotz, A. GP TANGER TI TUNING THE MAGNETOELECTRIC PROPERTIES WITH STRAIN IN EPITAXIAL CO0.9SN0.1FE2O4 THIN FILMS SO NANOCON 2014, 6TH INTERNATIONAL CONFERENCE LA English DT Proceedings Paper CT 6th NANOCON International Conference CY NOV 05-07, 2014 CL Brno, CZECH REPUBLIC SP TANGER Ltd, Czech Soc New Mat & Technologies, Reg Ctr Adv Technologies & Mat, Mat Res Soc Serbia, Norsk Materialteknisk Selskap DE Ferrite; substitution; magnetoelectric; magnetism; epitaxy ID MAGNETIC-PROPERTIES; FERRITES AB We have grown epitaxial Sn substituted cobalt ferrite thin films of various thicknesses on piezoelectric Pb(Mg1/3Nb2/(3))(0.72)Ti0.28O3 substrates and investigated the strain-induced changes of magnetic properties. All films described in this work have been deposited by pulsed laser deposition (PLD) from stoichiometric target of Co0.9Sn0.1Fe2O4. The lattice structure, crystallinity and orientation of the thin films were determined by X-ray diffraction analysis. The magnetization of thin films was measured for both, in-plane and out-of-plane configurations, using a superconductor quantum interference device (SQUID) magnetometer at 300 K. The measurements reveal that the magnetic anisotropy is altered by the strain imposed from the substrate upon application of an electric field. The magnetoelastic coupling is demonstrated by a change of the remanent magnetisation. However, we find that this strain effect is thickness dependent. The biggest strain effect is recorded for the thickest film (400nm) where an electric-field-controlled contraction of the substrate of 0.1% induces a relative change in magnetic moment of 9.3%. The relative change of the remanent magnetisation is reduced with decreasing film thickness and is smaller than 3% for the thinnest film (25nm). C1 [Rus, S. F.] Natl Inst Res & Dev Electrochem & Condensed Matte, Timisoara, Romania. [Herklotz, A.] Oak Ridge Natl Lab, Oak Ridge, TN USA. RP Rus, SF (reprint author), Natl Inst Res & Dev Electrochem & Condensed Matte, Timisoara, Romania. EM rusflorinastefania@gmail.com RI rus, florina stefania/E-8465-2016 OI rus, florina stefania/0000-0001-8505-0733 NR 18 TC 0 Z9 0 U1 0 U2 3 PU TANGER LTD PI SLEZSKA PA KELTICKOVA 62, SLEZSKA, OSTRAVA 710 00, CZECH REPUBLIC BN 978-80-87294-53-6 PY 2015 BP 766 EP 771 PG 6 WC Nanoscience & Nanotechnology; Physics, Applied SC Science & Technology - Other Topics; Physics GA BC1ZZ UT WOS:000350636300131 ER PT J AU Guo, Y Gu, D Jin, Z Du, PP Si, R Tao, J Xu, WQ Huang, YY Senanayake, S Song, QS Jia, CJ Schuth, F AF Guo, Yu Gu, Dong Jin, Zhao Du, Pei-Pei Si, Rui Tao, Jing Xu, Wen-Qian Huang, Yu-Ying Senanayake, Sanjaya Song, Qi-Sheng Jia, Chun-Jiang Schueth, Ferdi TI Uniform 2 nm gold nanoparticles supported on iron oxides as active catalysts for CO oxidation reaction: structure-activity relationship SO NANOSCALE LA English DT Article ID GAS SHIFT REACTION; CARBON-MONOXIDE; OXYGEN; TIO2; INCREASES; VACANCIES; NANORODS; AU-CEO2 AB Uniform Au nanoparticles (similar to 2 nm) with narrow size-distribution (standard deviation: 0.5-0.6 nm) supported on both hydroxylated (Fe_OH) and dehydrated iron oxide (Fe_O) have been prepared by either deposition-precipitation (DP) or colloidal-deposition (CD) methods. Different structural and textural characterizations were applied to the dried, calcined and used gold-iron oxide samples. Transmission electron microscopy (TEM) and high-resolution TEM (HRTEM) showed high homogeneity in the supported Au nanoparticles. The ex situ and in situ X-ray absorption fine structure (XAFS) characterization monitored the electronic and short-range local structure of active gold species. The synchrotron-based in situ X-ray diffraction (XRD), together with the corresponding temperature-programmed reduction by hydrogen (H2-TPR), indicated a structural evolution of the iron-oxide supports, correlating to their reducibility. An inverse order of catalytic activity between DP (Au/Fe_OH < Au/Fe_O) and CD (Au/Fe_OH > Au/Fe_O) was observed. Effective gold-support interaction results in a high activity for gold nanoparticles, locally generated by the sintering of dispersed Au atoms on the oxide support in the DP synthesis, while a hydroxylated surface favors the reactivity of externally introduced Au nanoparticles on Fe_OH support for the CD approach. This work reveals why differences in the synthetic protocol translate to differences in the catalytic performance of Au/FeOx catalysts with very similar structural characteristics in CO oxidation. C1 [Guo, Yu; Jin, Zhao; Song, Qi-Sheng; Jia, Chun-Jiang] Shandong Univ, Key Lab Colloid & Interface Chem, Key Lab Special Aggregated Mat, Sch Chem & Chem Engn, Jinan 250100, Peoples R China. [Gu, Dong; Schueth, Ferdi] Max Planck Inst Kohlenforsch, D-45470 Mulheim, Germany. [Du, Pei-Pei; Si, Rui; Huang, Yu-Ying] Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China. [Tao, Jing] Brookhaven Natl Lab, Condensed Matter Phys & Mat Sci Dept, Upton, NY 11973 USA. [Xu, Wen-Qian; Senanayake, Sanjaya] Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA. RP Si, R (reprint author), Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China. EM sirui@sinap.ac.cn; jiacj@sdu.edu.cn RI Gu, Dong/D-1940-2009; Schueth, Ferdi/B-1184-2017; Senanayake, Sanjaya/D-4769-2009 OI Gu, Dong/0000-0003-4600-4499; Senanayake, Sanjaya/0000-0003-3991-4232 FU National Science Foundation of China (NSFC) [21301107, 21373259, 11079005]; Shandong University [2014JC005]; Taishan Scholar project of Shandong Province (China); Chinese Academy of Sciences [XDA09030102]; Alexander von Humboldt Foundation; Max-Planck Society; DOE BES, by the Materials Sciences and Engineering Division [DE-AC02-98CH10886] FX Financial supported from the National Science Foundation of China (NSFC) (grant nos. 21301107, 21373259 and 11079005), Fundamental research funding of Shandong University (grant nos. 2014JC005), the Taishan Scholar project of Shandong Province (China), and the Hundred Talents project of the Chinese Academy of Sciences, the Strategic Priority Research Program of the Chinese Academy of Sciences (grant no. XDA09030102), the Alexander von Humboldt Foundation and the Max-Planck Society are greatly acknowledged. The work done at Brookhaven National Laboratory was supported by the DOE BES, by the Materials Sciences and Engineering Division under contract DE-AC02-98CH10886, and through the use of the Center for Functional Nanomaterials. NR 28 TC 15 Z9 15 U1 8 U2 121 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2040-3364 EI 2040-3372 J9 NANOSCALE JI Nanoscale PY 2015 VL 7 IS 11 BP 4920 EP 4928 DI 10.1039/c4nr06967f PG 9 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA CD4OA UT WOS:000351061700012 PM 25631762 ER PT J AU Yin, QY Gao, F Gu, ZY Stach, EA Zhou, GW AF Yin, Qiyue Gao, Fan Gu, Zhiyong Stach, Eric A. Zhou, Guangwen TI In situ visualization of metallurgical reactions in nanoscale Cu/Sn diffusion couples SO NANOSCALE LA English DT Article ID SN INTERMETALLIC COMPOUND; DEPENDENT MELTING PROPERTIES; LEAD-FREE SOLDERS; PB-FREE SOLDERS; CU-SN; INTERFACIAL REACTIONS; NANOTWINNED COPPER; VOID FORMATION; AG-CU/CU; GROWTH AB The Cu-Sn metallurgical soldering reaction in two-segmented Cu-Sn nanowires is studied by in situ transmission electron microscopy. By varying the relative lengths of Cu and Sn segments, we show that the metallurgical reaction results in a Cu-Sn solid solution for small Sn/Cu length ratio while Cu-Sn intermetallic compounds (IMCs) for larger Sn/Cu length ratios. Upon heating the nanowires to similar to 500 degrees C, two phase transformation pathways occur, eta-Cu6Sn5 -> epsilon-Cu3Sn -> delta-Cu41Sn11 for nanowires with a long Cu segment and eta-Cu6Sn5 -> epsilon-Cu3Sn -> gamma-Cu3Sn with a short Cu segment. The evolution of Kirkendall voids in the nanowires demonstrates that Cu diffuses faster than Sn in IMCs. Void growth results in the nanowire breakage that shuts off the inter-diffusion of Cu and Sn and thus leads to changes in the phase transformation pathway in the IMCs. C1 [Yin, Qiyue; Zhou, Guangwen] SUNY Binghamton, Dept Mech Engn, Binghamton, NY 13902 USA. [Yin, Qiyue; Zhou, Guangwen] SUNY Binghamton, Multidisciplinary Program Mat Sci & Engn, Binghamton, NY 13902 USA. [Gao, Fan; Gu, Zhiyong] Univ Massachusetts, Dept Chem Engn, Lowell, MA 01854 USA. [Stach, Eric A.] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA. RP Zhou, GW (reprint author), SUNY Binghamton, Dept Mech Engn, Binghamton, NY 13902 USA. EM gzhou@binghamton.edu RI Stach, Eric/D-8545-2011; OI Stach, Eric/0000-0002-3366-2153; Yin, Qiyue/0000-0002-6924-5116 FU National Science Foundation under NSF Collaborative Research Award [CMMI-1233806]; U.S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10886] FX This work was supported by the National Science Foundation under NSF Collaborative Research Award Grant CMMI-1233806. Research carried out in part at the Center for Functional Nanomaterials, Brookhaven National Laboratory, which is supported by the U.S. Department of Energy, Office of Basic Energy Sciences, under contract no. DE-AC02-98CH10886. NR 52 TC 8 Z9 8 U1 2 U2 29 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2040-3364 EI 2040-3372 J9 NANOSCALE JI Nanoscale PY 2015 VL 7 IS 11 BP 4984 EP 4994 DI 10.1039/c4nr06757f PG 11 WC Chemistry, Multidisciplinary; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied SC Chemistry; Science & Technology - Other Topics; Materials Science; Physics GA CD4OA UT WOS:000351061700021 PM 25692392 ER PT J AU Watkins, JD Roth, EA Lartey, M Albenze, E Zhong, MJ Luebke, DR Nulwala, HB AF Watkins, John D. Roth, Elliot A. Lartey, Michael Albenze, Erik Zhong, Mingjiang Luebke, David R. Nulwala, Hunaid B. TI Ionic liquid regioisomers: structure effect on the thermal and physical properties SO NEW JOURNAL OF CHEMISTRY LA English DT Article ID 1,2,3-TRIAZOLIUM-BASED POLY(IONIC LIQUID)S; CLICK CHEMISTRY POLYADDITION; ALKYL CHAIN-LENGTH; PHYSICOCHEMICAL PROPERTIES; TRANSPORT-PROPERTIES; CATION; WATER; SALTS AB A systematic study was performed on two triazolium ionic liquid isomers which included examination of thermal, physical, and electrochemical properties. It was found that a minor change in structure significantly influences physical and thermal properties of ionic liquids. C1 [Watkins, John D.; Roth, Elliot A.; Lartey, Michael; Albenze, Erik; Luebke, David R.; Nulwala, Hunaid B.] US DOE, Natl Energy Technol Lab, Pittsburgh, PA 15236 USA. [Albenze, Erik] URS Corp, South Pk, PA USA. [Zhong, Mingjiang] MIT, Dept Chem, Cambridge, MA 02139 USA. [Zhong, Mingjiang] MIT, Dept Chem Engn, Cambridge, MA 02139 USA. [Nulwala, Hunaid B.] Carnegie Mellon Univ, Dept Chem, Pittsburgh, PA 15213 USA. RP Nulwala, HB (reprint author), US DOE, Natl Energy Technol Lab, 626 Cochrans Mill Rd, Pittsburgh, PA 15236 USA. RI Zhong, Mingjiang/F-3470-2011; OI Zhong, Mingjiang/0000-0001-7533-4708; Nulwala, Hunaid/0000-0001-7481-3723 FU U.S. Department of Energy's National Energy Technology Laboratory [DE-FE0004000] FX This technical effort was performed in support of the U.S. Department of Energy's National Energy Technology Laboratory's on-going research on CO2 capture under the contract DE-FE0004000. NR 27 TC 3 Z9 3 U1 1 U2 12 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1144-0546 EI 1369-9261 J9 NEW J CHEM JI New J. Chem. PY 2015 VL 39 IS 3 BP 1563 EP 1566 DI 10.1039/c4nj01220h PG 4 WC Chemistry, Multidisciplinary SC Chemistry GA CD2HJ UT WOS:000350896000002 ER PT J AU Mitchell, E Jimenez, A Gupta, RK Gupta, BK Ramasamy, K Shahabuddin, M Mishra, SR AF Mitchell, Elias Jimenez, Ashley Gupta, Ram K. Gupta, Bipin Kumar Ramasamy, Karthik Shahabuddin, Mohammad Mishra, Sanjay R. TI Ultrathin porous hierarchically textured NiCo2O4-graphene oxide flexible nanosheets for high-performance supercapacitors SO NEW JOURNAL OF CHEMISTRY LA English DT Article ID HIGH SPECIFIC CAPACITANCE; NITROGEN-DOPED GRAPHENE; ELECTRODE MATERIALS; ELECTROCHEMICAL CAPACITORS; NANOSTRUCTURED CO3O4; FACILE SYNTHESIS; ENERGY-STORAGE; SOLAR-CELLS; NI FOAM; COMPOSITES AB The ultimate goal of supercapacitor research industries is to develop devices which could be used as flexible, portable, ultrathin and highly-efficient power sources. However, the bulk NiCo2O4 materials prevent the achievement of high energy density as well as immense rate performance due to the limited electroactive surface area. In this work, we proposed a new breakthrough strategy to develop highly porous hierarchical flexible nanosheets of NiCo2O4-graphene oxide (NiCo2O4-GO) on nickel foam by a facile electrochemical deposition method. The morphogenesis of the NiCo2O4-GO hybrid nanostructure-based electrode exhibits hierarchical porous flexible nanosheet-like structures. The electrochemical properties of these electrodes were investigated by cyclic voltammetry and galvanostatic charge-discharge measurements in 3 M KOH electrolyte. The obtained results exhibit that this new hybrid nanostructure has a specific capacitance of 1078 F g(-1) at a discharge current of 1 mA with great cyclic stability. These excellent capacitive performances of NiCo2O4-GO can be attributed to its hierarchical porous nanosheet-like unique structure. This unique structure provides efficient ion transport that is highly desirable for superior rate capability and excellent cycling stability. Hence, our method provides a promising facile and binder-free nanostructure electrode for next generation high-performance supercapacitor applications. C1 [Mitchell, Elias; Jimenez, Ashley; Gupta, Ram K.] Pittsburg State Univ, Dept Chem, Pittsburg, KS 66762 USA. [Gupta, Bipin Kumar] CSIR, Natl Phys Lab, New Delhi 110012, India. [Ramasamy, Karthik] Los Alamos Natl Lab, Ctr Integrated Nanotechnol, Los Alamos, NM 87545 USA. [Shahabuddin, Mohammad; Mishra, Sanjay R.] Univ Memphis, Dept Phys, Memphis, TN 38152 USA. RP Gupta, RK (reprint author), Pittsburg State Univ, Dept Chem, 1701 S Broadway, Pittsburg, KS 66762 USA. EM ramguptamsu@gmail.com FU Pittsburg State University; National Science Foundation [EPS-0903806] FX Authors wish to thank Pittsburg State University for providing financial support. This material is based upon work supported by the National Science Foundation under Award No. EPS-0903806 and matching support from the State of Kansas through the Kansas Board of Regents. Authors also wish to thank Integrated Microscopy Center at the University of Memphis for providing FE-SEM facility. NR 63 TC 14 Z9 14 U1 11 U2 90 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1144-0546 EI 1369-9261 J9 NEW J CHEM JI New J. Chem. PY 2015 VL 39 IS 3 BP 2181 EP 2187 DI 10.1039/c4nj02110j PG 7 WC Chemistry, Multidisciplinary SC Chemistry GA CD2HJ UT WOS:000350896000065 ER PT J AU Zhao, JL Tomiyasu, H Ni, XL Zeng, X Elsegood, MRJ Redshaw, C Rahman, S Georghiou, PE Teat, SJ Yamato, T AF Zhao, Jiang-Lin Tomiyasu, Hirotsugu Ni, Xin-Long Zeng, Xi Elsegood, Mark R. J. Redshaw, Carl Rahman, Shofiur Georghiou, Paris E. Teat, Simon J. Yamato, Takehiko TI The first study about the relationship between the extractability of thiacalix[4]arene derivatives and the position of the coordination binding sites SO ORGANIC & BIOMOLECULAR CHEMISTRY LA English DT Article ID BEARING IMIDAZOLE UNITS; INCLUSION PROPERTIES; DICHROMATE ANION; MAGNETITE NANOPARTICLES; EXTRACTION PROPERTIES; CYCLIC POLYETHERS; METAL-SALTS; COMPLEXES; TRANSITION; ALKALI AB Three organic ionophores (2-4) based on the p-tert-butylthiacalix[4] arene backbone, blocked in the 1,3-alternate conformation, bearing two pyridyl coordinating moieties (ortho for 2, meta for 3 and para for 4), have been synthesized and characterized in the solid state. The solvent extraction experiments with the metal ions showed that the ability of these derivatives to complex with Ag+ appeared to be largely dependent on the position of the nitrogen atoms of the pyridyl ring. Two different complexation modes have been confirmed by H-1 NMR titration. Ionophore 2 armed with two pyridyl moieties, complexed with Ag+ cation through N center dot center dot center dot Ag+center dot center dot center dot S interactions; however, ionophore 3 and ionophore 4 complexed with Ag+ through metal-nitrogen (N center dot center dot center dot Ag+) interactions. The DFT computational studies were consistent with the experimental findings. These findings will provide us with an important rule to design an appropriate thiacalix[4] arene ionophore in the future. Another study on the possibility for application of ionophores 2-4 for the treatment of waste water containing Cr(VI) and Cr(III), showed that ionophore 3 was useful in the application of the solvent extraction method in selective treatment of waste water containing Cr(VI) and Cr(III) prior to discharge. C1 [Zhao, Jiang-Lin; Tomiyasu, Hirotsugu; Yamato, Takehiko] Saga Univ, Fac Sci & Engn, Dept Appl Chem, Saga 8408502, Japan. [Ni, Xin-Long; Zeng, Xi] Guizhou Univ, Dept Key Lab Macrocycl & Supramol Chem Guizhou Pr, Guiyang 550025, Guizhou, Peoples R China. [Elsegood, Mark R. J.] Univ Loughborough, Dept Chem, Loughborough LE11 3TU, Leics, England. [Redshaw, Carl] Univ Hull, Dept Chem, Kingston Upon Hull HU6 7RX, Yorks, England. [Rahman, Shofiur; Georghiou, Paris E.] Mem Univ Newfoundland, Dept Chem, St John, NF A1B 3X7, Canada. [Teat, Simon J.] Berkeley Lab, ALS, Berkeley, CA 94720 USA. RP Yamato, T (reprint author), Saga Univ, Fac Sci & Engn, Dept Appl Chem, Honjo Machi 1, Saga 8408502, Japan. EM yamatot@cc.saga-u.ac.jp RI Redshaw, Carl/C-5644-2009 OI Redshaw, Carl/0000-0002-2090-1688 FU OTEC at Saga University; International Cooperation Projects of Guizhou Province, The Royal Society of Chemistry [20137002]; EPSRC; Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231] FX This work was performed under the Cooperative Research Program of "Network Joint Research Center for Materials and Devices (Institute for Materials Chemistry and Engineering, Kyushu University)". We would like to thank the OTEC at Saga University and the International Cooperation Projects of Guizhou Province (no. 20137002), The Royal Society of Chemistry for financial support and the EPSRC for an overseas travel grant to C.R. 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 47 TC 3 Z9 3 U1 1 U2 9 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1477-0520 EI 1477-0539 J9 ORG BIOMOL CHEM JI Org. Biomol. Chem. PY 2015 VL 13 IS 11 BP 3476 EP 3483 DI 10.1039/c4ob02393e PG 8 WC Chemistry, Organic SC Chemistry GA CD4OK UT WOS:000351062700039 PM 25666118 ER PT S AU Aytac, Y Olson, BV Kim, JK Shaner, EA Hawkins, SD Klem, JF Flatte, ME Boggess, TF AF Aytac, Y. Olson, B. V. Kim, J. K. Shaner, E. A. Hawkins, S. D. Klem, J. F. Flatte, M. E. Boggess, T. F. BE Razeghi, M Tournie, E Brown, GJ TI Temperature dependent carrier lifetime measurements of InAs/InAsSb T2SLs SO QUANTUM SENSING AND NANOPHOTONIC DEVICES XII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Quantum Sensing and Nanophotonic Devices XII CY FEB 08-12, 2015 CL San Francisco, CA SP SPIE DE InAs/InAsSb; Lifetime; T2SLs ID SUPERLATTICES AB Temperature dependent measurements of carrier recombination rates using a time-resolved pump-probe technique are reported for mid-wave infrared InAs/InAsSb type-2 superlattices (T2SLs). By engineering the layer widths and alloy compositions a 16 K band-gap of similar to 235 +/- 10meV was achieved for four doped and five undoped T2SLs. Carrier lifetimes were determined by fitting lifetime models of Shockley-Read-Hall (SRH), radiative, and Auger recombination processes simultaneously to the temperature and excess carrier density dependent data. The contribution of each recombination process at a given temperature is identified and the total lifetime is determined over a range of excess carrier densities. The minority carrier and Auger lifetimes were observed to increase with increasing antimony content and decreasing layer thickness for the undoped T2SLs. It is hypothesized that a reduction in SRH recombination centers or a shift in the SRH defect energy relative to the T2SL band edges is the cause of this increase in the SRH minority carrier lifetime. The lower Auger coefficients are attributed to a reduced number of final Auger states in the SL samples with greater antimony content. An Auger limited minority carrier lifetime is observed for the doped T2SLs, and it is found to be a factor of ten shorter than for undoped T2SLs. The Auger rates for all the InAs/InAsSb T2SLs were significantly larger than those previously reported for InAs/GaSb T2SLs. C1 [Aytac, Y.; Flatte, M. E.; Boggess, T. F.] Univ Iowa, Dept Phys & Astron, Iowa City, IA 52242 USA. [Aytac, Y.; Flatte, M. E.; Boggess, T. F.] Univ Iowa, Opt Sci & Technol Ctr, Iowa City, IA 52242 USA. [Olson, B. V.; Kim, J. K.; Shaner, E. A.; Hawkins, S. D.; Klem, J. F.] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Aytac, Y (reprint author), Univ Iowa, Dept Phys & Astron, Iowa City, IA 52242 USA. EM yigit-aytac@uiowa.edu; benolso@sandia.gov NR 18 TC 1 Z9 1 U1 4 U2 20 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-1-62841-460-8 J9 PROC SPIE PY 2015 VL 9370 AR 93700J DI 10.1117/12.2077753 PG 8 WC Engineering, Electrical & Electronic; Optics; Physics, Applied SC Engineering; Optics; Physics GA BC1NA UT WOS:000350275500011 ER PT S AU Haglund, RF Weiss, SM Appavoo, K AF Haglund, Richard F., Jr. Weiss, Sharon M. Appavoo, Kannatassen BE Razeghi, M Tournie, E Brown, GJ TI Photonic and plasmonic modulators based on optical switching in VO2 SO QUANTUM SENSING AND NANOPHOTONIC DEVICES XII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Quantum Sensing and Nanophotonic Devices XII CY FEB 08-12, 2015 CL San Francisco, CA SP SPIE DE Vanadium dioxide; silicon; insulator-to-metal transition; gold plasmon resonance; hybrid ring resonator; heterodimer nanomodulator; electron beam lithography; ultrafast phase transition ID PULSED-LASER DEPOSITION; METAL-INSULATOR TRANSITIONS; DIOXIDE THIN-FILMS; PHASE-TRANSITION; ACTIVE PLASMONICS; SILICON; SEMICONDUCTOR; NANOPARTICLES; NANOANTENNA; TEMPERATURE AB Researchers all over the world are competing in a technology-driven quest to develop the next generation of ultrasmall, low-power photonic and plasmonic devices. One route to this objective involves hybrid structures that incorporate a phase-changing material into the structure, creating a nanocomposite material in which the optical response of a plasmonic or photonic structure is modulated by a change in phase, crystallinity or dielectric function induced by thermal, optical or electrical stimulus. Vanadium dioxide (VO2) has been considered as a potential electro-optic switching material for electronic and photonic applications ever since its semiconductor-to-metal transition (SMT) was first described half a century ago. This review describes the application of vanadium dioxide as the switching element in (i) a hybrid silicon ring resonator and (ii) a polarization-sensitive, multifunctional plasmonic modulator in the form of a nanoscale heterodimer. As is now widely known, the SMT in VO2 is also accompanied by a structural phase transition (SPT) from the M1 (monoclinic) to a rutile (tetragonal, R) crystalline form that was believed to prevent a fast recovery after switching. However, recent research has shown that this picture is oversimplified, and that there is a monoclinic metallic state that enables true ultrafast switching. That understanding, in turn, is leading to new concepts in developing hybrid nanocomposites that incorporate VO2 in silicon photonics and plasmonic modulators, enabling the construction of ultrafast optical switches, modulators and memory elements. C1 [Haglund, Richard F., Jr.] Vanderbilt Univ, Dept Phys & Astron, Nashville, TN 37235 USA. [Weiss, Sharon M.] Vanderbilt Univ, Dept Elect & Comp Sci, Nashville, TN 37235 USA. [Appavoo, Kannatassen] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11793 USA. RP Haglund, RF (reprint author), Vanderbilt Univ, Dept Phys & Astron, Nashville, TN 37235 USA. NR 60 TC 0 Z9 0 U1 3 U2 30 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-1-62841-460-8 J9 PROC SPIE PY 2015 VL 9370 AR 93701C DI 10.1117/12.2083422 PG 12 WC Engineering, Electrical & Electronic; Optics; Physics, Applied SC Engineering; Optics; Physics GA BC1NA UT WOS:000350275500037 ER PT S AU Mitrofanov, O Dominec, F Kuzel, P Reno, JL Brener, I Chung, UC Elissalde, C Maglione, M Mounaix, P AF Mitrofanov, Oleg Dominec, Filip Kuzel, Petr Reno, John L. Brener, Igal Chung, U-Chan Elissalde, Cathy Maglione, Mario Mounaix, Patrick BE Razeghi, M Tournie, E Brown, GJ TI Magnetic dipole and electric dipole resonances in TiO2 microspheres at terahertz frequencies SO QUANTUM SENSING AND NANOPHOTONIC DEVICES XII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Quantum Sensing and Nanophotonic Devices XII CY FEB 08-12, 2015 CL San Francisco, CA SP SPIE DE Terahertz; metamaterials; dielectric resonator; near-field imaging; Mie mode; TiO2 micro-sphere; Fano line-shape; THz spectroscopy AB In a non-magnetic dielectric sphere of high-permittivity (epsilon > 20), effective magnetic response occurs as a result of the 1st Mie mode, known as the magnetic dipole resonance. This resonance produces a similar effect as split ring resonators, making it possible to use dielectric spheres as metamaterial components. In the terahertz (THz) part of the spectrum, where dielectrics with epsilon similar to 100 can be found, all-dielectric metamaterials can potentially reduce absorption and provide isotropic and polarization-independent properties. In this contribution, we discuss TiO2 micro-spheres, similar to 1/10 of the wavelength in diameter. Such spheres are expected to support the magnetic and electric dipole resonances. To detect these resonances in a single TiO2 microsphere we use THz near-field microscopy with the sub-wavelength size aperture probe. This method allows detection of Mie resonances in single sub-wavelength spheres. Fano-type line-shape is observed in the near-field amplitude and phase spectra. The narrow line-width of the magnetic resonance and the sub-wavelength size of the TiO2 microspheres make them excellent candidates for realizing low-loss THz metamaterials. C1 [Mitrofanov, Oleg] UCL, Dept Elect & Elect Engn, London WC1E 7JE, England. [Mitrofanov, Oleg; Reno, John L.; Brener, Igal] Sandia Natl Labs, Ctr Integrated Nanotechnol, Albuquerque, NM 87185 USA. [Dominec, Filip; Kuzel, Petr] Acad Sci Czech Republic, Prague 18221, Czech Republic. [Reno, John L.; Brener, Igal] Sandia Natl Labs, Albuquerque, NM 87185 USA. [Chung, U-Chan; Elissalde, Cathy; Maglione, Mario] Univ Bordeaux, CNRS, ICMCB, UPR 9048, F-33600 Pessac, France. [Mounaix, Patrick] Univ Bordeaux, CNRS, UMR 5798, LOMA, F-33405 Talence, France. RP Mitrofanov, O (reprint author), UCL, Dept Elect & Elect Engn, London WC1E 7JE, England. EM o.mitrofanov@ucl.ac.uk RI Kuzel, Petr/G-6006-2014; Mitrofanov, Oleg/C-1938-2008 OI Mitrofanov, Oleg/0000-0003-3510-2675 NR 5 TC 0 Z9 0 U1 4 U2 24 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-1-62841-460-8 J9 PROC SPIE PY 2015 VL 9370 AR 937005 DI 10.1117/12.2079734 PG 6 WC Engineering, Electrical & Electronic; Optics; Physics, Applied SC Engineering; Optics; Physics GA BC1NA UT WOS:000350275500002 ER PT S AU Phillips, MC Taubman, MS Kriesel, J AF Phillips, Mark C. Taubman, Matthew S. Kriesel, Jason BE Razeghi, M Tournie, E Brown, GJ TI Use of external cavity quantum cascade laser compliance voltage in real-time trace gas sensing of multiple chemicals SO QUANTUM SENSING AND NANOPHOTONIC DEVICES XII SE Proceedings of SPIE LA English DT Proceedings Paper CT Conference on Quantum Sensing and Nanophotonic Devices XII CY FEB 08-12, 2015 CL San Francisco, CA SP SPIE DE Infrared spectroscopy; quantum cascade laser; tunable laser; gas sensing ID ATMOSPHERIC AMMONIA MEASUREMENTS; OPEN-PATH; SPECTROSCOPY; SENSOR; SPECTROMETER; CALIBRATION; EMISSION AB We describe a prototype trace gas sensor designed for real-time detection of multiple chemicals. The sensor uses an external cavity quantum cascade laser (ECQCL) swept over its tuning range of 940-1075 cm-1 (9.30-10.7 mu m) at a 10 Hz repetition rate. The sensor was designed for operation in multiple modes, including gas sensing within a multi-pass Heriott cell and intracavity absorption sensing using the ECQCL compliance voltage. In addition, the ECQCL compliance voltage was used to reduce effects of long-term drifts in the ECQCL output power. The sensor was characterized for noise, drift, and detection of chemicals including ammonia, methanol, ethanol, isopropanol, Freon-134a, Freon-152a, and diisopropyl methylphosphonate (DIMP). We also present use of the sensor for mobile detection of ammonia downwind of cattle facilities, in which concentrations were recorded at 1-s intervals. C1 [Phillips, Mark C.; Taubman, Matthew S.] Pacific NW Natl Lab, Richland, WA 99352 USA. [Kriesel, Jason] OKSI, Torrance, CA 90502 USA. RP Phillips, MC (reprint author), Pacific NW Natl Lab, POB 999, Richland, WA 99352 USA. NR 29 TC 2 Z9 2 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 978-1-62841-460-8 J9 PROC SPIE PY 2015 VL 9370 AR 93700Z DI 10.1117/12.2080852 PG 14 WC Engineering, Electrical & Electronic; Optics; Physics, Applied SC Engineering; Optics; Physics GA BC1NA UT WOS:000350275500024 ER PT J AU Li, WB Klein, W Blanchardon, E Puncher, M Leggett, RW Oeh, U Breustedt, B Nosske, D Lopez, MA AF Li, W. B. Klein, W. Blanchardon, E. Puncher, M. Leggett, R. W. Oeh, U. Breustedt, B. Nosske, D. Lopez, M. A. TI Parameter uncertainty analysis of a biokinetic model of caesium SO RADIATION PROTECTION DOSIMETRY LA English DT Article ID ICRPS DOSE COEFFICIENTS; INTERNAL DOSIMETRY; TRACT MODEL; RELIABILITY; ZIRCONIUM; PREDICTIONS; EXPOSURE; MEMBERS; HUMANS AB Parameter uncertainties for the biokinetic model of caesium (Cs) developed by Leggett et al. were inventoried and evaluated. The methods of parameter uncertainty analysis were used to assess the uncertainties of model predictions with the assumptions of model parameter uncertainties and distributions. Furthermore, the importance of individual model parameters was assessed by means of sensitivity analysis. The calculated uncertainties of model predictions were compared with human data of Cs measured in blood and in the whole body. It was found that propagating the derived uncertainties in model parameter values reproduced the range of bioassay data observed in human subjects at different times after intake. The maximum ranges, expressed as uncertainty factors (UFs) (defined as a square root of ratio between 97.5th and 2.5th percentiles) of blood clearance, whole-body retention and urinary excretion of Cs predicted at earlier time after intake were, respectively: 1.5, 1.0 and 2.5 at the first day; 1.8, 1.1 and 2.4 at Day 10 and 1.8, 2.0 and 1.8 at Day 100; for the late times (1000 d) after intake, the UFs were increased to 43, 24 and 31, respectively. The model parameters of transfer rates between kidneys and blood, muscle and blood and the rate of transfer from kidneys to urinary bladder content are most influential to the blood clearance and to the whole-body retention of Cs. For the urinary excretion, the parameters of transfer rates from urinary bladder content to urine and from kidneys to urinary bladder content impact mostly. The implication and effect on the estimated equivalent and effective doses of the larger uncertainty of 43 in whole-body retention in the later time, say, after Day 500 will be explored in a successive work in the framework of EURADOS. C1 [Li, W. B.; Oeh, U.] German Res Ctr Environm Hlth GmbH, Helmholtz Zentrum Munchen, HMGU Res Unit Med Radiat Phys & Diagnost, D-85764 Neuherberg, Germany. [Klein, W.] Karlsruhe Inst Technol, KIT Inst Nucl Waste Disposal, D-76344 Eggenstein Leopoldshafen, Germany. [Blanchardon, E.] PRP HOM SDI LEDI, IRSN Internal Dose Assessment Lab, F-92262 Fontenay Aux Roses, France. [Puncher, M.] Publ Hlth England, Ctr Radiat Chem & Environm Hazards, PHE Dept Toxicol, Didcot OX11 0RQ, Oxon, England. [Leggett, R. W.] Oak Ridge Natl Lab, Div Environm Sci, Oak Ridge, TN 37831 USA. [Breustedt, B.] Karlsruhe Inst Technol, KIT Safety Management, D-76344 Eggenstein Leopoldshafen, Germany. [Nosske, D.] BfS Dept Radiat Protect & Hlth, D-85764 Oberschleissheim, Germany. [Lopez, M. A.] CIEMAT Dosimetria Interna, Dept Medio Ambiente, Madrid 28040, Spain. RP Li, WB (reprint author), German Res Ctr Environm Hlth GmbH, Helmholtz Zentrum Munchen, HMGU Res Unit Med Radiat Phys & Diagnost, D-85764 Neuherberg, Germany. EM wli@helmholtz-muenchen.de FU EURADOS e.V.; German Federal Ministry of Education and Research (BMBF) [NUK002B, 02NUK015B] FX This work was supported by the EURADOS e.V. (www.eurados.org) and was partially supported by the German Federal Ministry of Education and Research (BMBF) with contract number NUK002B (KVSFI) and 02NUK015B (KVSF II). NR 47 TC 5 Z9 5 U1 1 U2 5 PU OXFORD UNIV PRESS PI OXFORD PA GREAT CLARENDON ST, OXFORD OX2 6DP, ENGLAND SN 0144-8420 EI 1742-3406 J9 RADIAT PROT DOSIM JI Radiat. Prot. Dosim. PD JAN PY 2015 VL 163 IS 1 BP 37 EP 57 DI 10.1093/rpd/ncu055 PG 21 WC Environmental Sciences; Public, Environmental & Occupational Health; Nuclear Science & Technology; Radiology, Nuclear Medicine & Medical Imaging SC Environmental Sciences & Ecology; Public, Environmental & Occupational Health; Nuclear Science & Technology; Radiology, Nuclear Medicine & Medical Imaging GA CC1QK UT WOS:000350116300005 PM 24743755 ER PT J AU Chen, Y Jakeman, J Gittelson, C Xiu, DB AF Chen, Yi Jakeman, John Gittelson, Claude Xiu, Dongbin TI LOCAL POLYNOMIAL CHAOS EXPANSION FOR LINEAR DIFFERENTIAL EQUATIONS WITH HIGH DIMENSIONAL RANDOM INPUTS SO SIAM JOURNAL ON SCIENTIFIC COMPUTING LA English DT Article DE generalized polynomial chaos; domain decomposition; stochastic differential equation; uncertainty quantification ID FINITE-ELEMENTS; EPISTEMIC UNCERTAINTY; NUMERICAL APPROACH; COLLOCATION METHOD; ELLIPTIC PROBLEMS; DIFFUSION; QUANTIFICATION; DECOMPOSITION; SCHEMES AB In this paper we present a localized polynomial chaos expansion for partial differential equations (PDE) with random inputs. In particular, we focus on time independent linear stochastic problems with high dimensional random inputs, where the traditional polynomial chaos methods, and most of the existing methods, incur prohibitively high simulation cost. The local polynomial chaos method employs a domain decomposition technique to approximate the stochastic solution locally. In each subdomain, a subdomain problem is solved independently and, more importantly, in a much lower dimensional random space. In a postprocesing stage, accurate samples of the original stochastic problems are obtained from the samples of the local solutions by enforcing the correct stochastic structure of the random inputs and the coupling conditions at the interfaces of the subdomains. Overall, the method is able to solve stochastic PDEs in very large dimensions by solving a collection of low dimensional local problems and can be highly efficient. In this paper we present the general mathematical framework of the methodology and use numerical examples to demonstrate the properties of the method. C1 [Chen, Yi] Purdue Univ, Dept Math, W Lafayette, IN 47907 USA. [Jakeman, John] Sandia Natl Labs, Albuquerque, NM 87185 USA. [Gittelson, Claude] ETH, CH-8092 Zurich, Switzerland. [Xiu, Dongbin] Univ Utah, Dept Math & Sci Comp & Imaging Inst, Salt Lake City, UT 84112 USA. RP Xiu, DB (reprint author), Univ Utah, Dept Math & Sci Comp & Imaging Inst, Salt Lake City, UT 84112 USA. EM chen411@purdue.edu; jdjakem@sandia.gov; claude.gittelson@sam.math.ethz.ch; dongbin.xiu@utah.edu FU AFOSR; DOE; NSF; U.S. Department of Energy, Office of Science, Office of Advanced Scientific Computing Research, Applied Mathematics program; U.S. Department of Energy National Nuclear Security Administration [DE-AC04-94AL85000] FX This work was partly supported by AFOSR, DOE, and NSF.; This author's work was supported by the U.S. Department of Energy, Office of Science, Office of Advanced Scientific Computing Research, Applied Mathematics program. Sandia National Laboratories is a multiprogram laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy National Nuclear Security Administration under contract DE-AC04-94AL85000. NR 40 TC 5 Z9 5 U1 0 U2 1 PU SIAM PUBLICATIONS PI PHILADELPHIA PA 3600 UNIV CITY SCIENCE CENTER, PHILADELPHIA, PA 19104-2688 USA SN 1064-8275 EI 1095-7197 J9 SIAM J SCI COMPUT JI SIAM J. Sci. Comput. PY 2015 VL 37 IS 1 BP A79 EP A102 DI 10.1137/140970100 PG 24 WC Mathematics, Applied SC Mathematics GA CD6PA UT WOS:000351210200004 ER PT J AU Osei-Kuffuor, D Li, RP Saad, Y AF Osei-Kuffuor, Daniel Li, Ruipeng Saad, Yousef TI MATRIX REORDERING USING MULTILEVEL GRAPH COARSENING FOR ILU PRECONDITIONING SO SIAM JOURNAL ON SCIENTIFIC COMPUTING LA English DT Article DE incomplete factorization preconditioners; algebraic preconditioners; ILU preconditioners; sparse matrix reordering; multilevel graph coarsening ID INCOMPLETE LU FACTORIZATIONS; DEGREE ORDERING ALGORITHM; SMOOTHED AGGREGATION; COMPATIBLE RELAXATION; NONSYMMETRIC PROBLEMS; CONJUGATE GRADIENTS; HELMHOLTZ-EQUATION; ITERATIVE SOLUTION; ELLIPTIC PROBLEMS; SPARSE MATRICES AB Incomplete LU factorization (ILU) techniques are a well-known class of preconditioners, often used in conjunction with Krylov accelerators for the iterative solution of linear systems of equations. However, for certain problems, ILU factorizations can yield factors that are unstable and in some cases quite dense. Reordering techniques based on permuting the matrix prior to performing the factorization have been shown to improve the quality of the factorization, and the resulting preconditioner. In this paper, we examine the effect of reordering techniques based on multilevel graph coarsening ideas on one-level ILU factorizations, such as the level-based ILU(k) or the dual threshold ILUT algorithms. We consider an aggregation-based coarsening idea that implements two main coarsening frameworks-a top-down approach, and a bottom-up approach-each utilizing one of two different strategies to select the next-level coarse graph. Numerical results are presented to support our findings. C1 [Osei-Kuffuor, Daniel] Lawrence Livermore Natl Lab, Ctr Appl Sci Comp, Livermore, CA 94551 USA. [Li, Ruipeng; Saad, Yousef] Univ Minnesota, Dept Comp Sci & Engn, Minneapolis, MN 55455 USA. RP Osei-Kuffuor, D (reprint author), Lawrence Livermore Natl Lab, Ctr Appl Sci Comp, L-561, Livermore, CA 94551 USA. EM oseikuffuor1@llnl.gov; rli@cs.umn.edu; saad@cs.umn.edu FU U.S. Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07NA27344]; NSF [NSF/DMS-1216366]; Minnesota Supercomputer Institute FX The work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under contract DE-AC52-07NA27344.; Work supported by NSF under grant NSF/DMS-1216366 and by the Minnesota Supercomputer Institute. NR 75 TC 1 Z9 1 U1 0 U2 3 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 2015 VL 37 IS 1 BP A391 EP A419 DI 10.1137/130936610 PG 29 WC Mathematics, Applied SC Mathematics GA CD6PA UT WOS:000351210200017 ER PT J AU Tumblin, R Ahrens, P Hartse, S Robey, RW AF Tumblin, Rebecka Ahrens, Peter Hartse, Sara Robey, Robert W. TI PARALLEL COMPACT HASH ALGORITHMS FOR COMPUTATIONAL MESHES SO SIAM JOURNAL ON SCIENTIFIC COMPUTING LA English DT Article DE hashing; compact hash; parallel computing; AMR; GPU; cell-based adoptive mesh refinement ID UNIVERSAL CLASSES; SCATTER STORAGE; FLUID-DYNAMICS; REFINEMENT; EQUATIONS; CODE AB We employ compact hashing and the discrete properties of computational meshes to optimize spatial operations in scientific computing applications. Our target is to develop highly parallel compact hashing methods suitable for the fine-grained parallelism of GPU and MIC architectures that will scale to the next generation of computing systems. As a model, we apply spatial hashing methods to the problem of determining neighbor elements in adaptive mesh refinement (AMR) schemes. By applying memory savings techniques, we extend the perfect spatial hash algorithm to a compact hash by compressing the resulting sparse data structures. Using compact hashing and specific memory optimizations, we increase the range of problems that can benefit from our ideal O(n) algorithms. The spatial hash methods are tested and compared across a variety of architectures on both a randomly generated sample mesh and an existing cell-based AMR shallow-water hydrodynamics scheme. We demonstrate consistent speed-up and increased performance across every device tested and explore the ubiquitous application of spatial hashing in scientific computing. C1 [Tumblin, Rebecka; Ahrens, Peter; Hartse, Sara; Robey, Robert W.] Los Alamos Natl Lab, Eulerian Applicat Grp XCP 2, Los Alamos, NM 87545 USA. [Tumblin, Rebecka] Univ Oregon, Inst Theoret Sci, Eugene, OR 97403 USA. [Ahrens, Peter] Univ Calif Berkeley, Dept Elect Engn & Comp Sci, Berkeley, CA 94709 USA. [Hartse, Sara] Brown Univ, Dept Comp Sci, Providence, RI 02912 USA. RP Tumblin, R (reprint author), Los Alamos Natl Lab, Eulerian Applicat Grp XCP 2, Los Alamos, NM 87545 USA. EM rtumblin@uoregon.edu; ptrahrens@gmail.com; sara.hartse@gmail.com; brobey@lanl.gov FU Los Alamos National Laboratory Director's Office; National Nuclear Security Administration of the U.S. Department of Energy [DE-AC52-06NA25396] FX This work was partially supported by the Los Alamos National Laboratory Director's Office. 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. NR 26 TC 0 Z9 0 U1 2 U2 6 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 2015 VL 37 IS 1 BP C31 EP C53 DI 10.1137/13093371X PG 23 WC Mathematics, Applied SC Mathematics GA CD6PA UT WOS:000351210200030 ER PT S AU Agranovsky, A Camp, D Joy, KI Childs, H AF Agranovsky, Alexy Camp, David Joy, Kenneth I. Childs, Hank BE Kao, DL Hao, MC Livingston, MA Wischgoll, T TI Subsampling-Based Compression and Flow Visualization SO VISUALIZATION AND DATA ANALYSIS 2015 SE Proceedings of SPIE LA English DT Proceedings Paper CT 22nd Annual IS and T/SPIE Conference on Visualization and Data Analysis (VDA) CY FEB 09-11, 2015 CL San Francisco, CA SP Soc Imaging Sci & Technol, SPIE, Kitware Inc DE In Situ; Sub-Sampling; Compression; Adaptive Budget; Flow Visualization ID QUERY-DRIVEN VISUALIZATION; TIME-VARYING DATA; 2D VECTOR-FIELDS AB As computational capabilities increasingly outpace disk speeds on leading supercomputers, scientists will, in turn, be increasingly unable to save their simulation data at its native resolution. One solution to this problem is to compress these data sets as they are generated and visualize the compressed results afterwards. We explore this approach, specifically subsampling velocity data and the resulting errors for particle advection-based flow visualization. We compare three techniques: random selection of subsamples, selection at regular locations corresponding to multi-resolution reduction, and introduce a novel technique for informed selection of subsamples. Furthermore, we explore an adaptive system which exchanges the subsampling budget over parallel tasks, to ensure that subsampling occurs at the highest rate in the areas that need it most. We perform supercomputing runs to measure the effectiveness of the selection and adaptation techniques. Overall, we find that adaptation is very effective, and, among selection techniques, our informed selection provides the most accurate results, followed by the multi-resolution selection, and with the worst accuracy coming from random subsamples. C1 [Agranovsky, Alexy; Joy, Kenneth I.] Univ Calif Davis, Davis, CA 95616 USA. [Agranovsky, Alexy; Camp, David; Childs, Hank] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA. [Childs, Hank] Univ Oregon, Eugene, OR 97403 USA. RP Agranovsky, A (reprint author), Univ Calif Davis, 1 Shields Ave, Davis, CA 95616 USA. EM aagranovsky@ucdavis.edu; dcamp@lbl.gov; kijoy@ucdavis.edu; hchilds@uoregon.edu NR 26 TC 0 Z9 0 U1 0 U2 1 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-1-62841-487-5 J9 PROC SPIE PY 2015 VL 9397 AR 93970J DI 10.1117/12.2083251 PG 14 WC Computer Science, Theory & Methods; Engineering, Electrical & Electronic; Optics SC Computer Science; Engineering; Optics GA BC1NC UT WOS:000350276200018 ER PT S AU Nugent, P Cao, Y Kasliwal, M AF Nugent, Peter Cao, Yi Kasliwal, Mansi BE Kao, DL Hao, MC Livingston, MA Wischgoll, T TI The Palomar Transient Factory SO VISUALIZATION AND DATA ANALYSIS 2015 SE Proceedings of SPIE LA English DT Proceedings Paper CT 22nd Annual IS and T/SPIE Conference on Visualization and Data Analysis (VDA) CY FEB 09-11, 2015 CL San Francisco, CA SP Soc Imaging Sci & Technol, SPIE, Kitware Inc DE Image Processing; Transient Detection; Machine Learning; Workflows ID DISCOVERY; REDSHIFT AB Astrophysics is transforming from a data-starved to a data-swamped discipline, fundamentally changing the nature of scientific inquiry and discovery. New technologies are enabling the detection, transmission, and storage of data of hitherto unimaginable quantity and quality across the electromagnetic, gravity and particle spectra. The observational data obtained during this decade alone will supersede everything accumulated over the preceding four thousand years of astronomy. Currently there are 4 large-scale photometric and spectroscopic surveys underway, each generating and/or utilizing hundreds of terabytes of data per year. Some will focus on the static universe while others will greatly expand our knowledge of transient phenomena. Maximizing the science from these programs requires integrating the processing pipeline with high-performance computing resources. These are coupled to large astrophysics databases while making use of machine learning algorithms with near real-time turnaround. Here we present an overview of one of these programs, the Palomar Transient Factory (PTF). We will cover the processing and discovery pipeline we developed at LBNL and NERSC for it and several of the great discoveries made during the 4 years of observations with PTF. C1 [Nugent, Peter] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Computat Cosmol Ctr, Berkeley, CA 94720 USA. [Nugent, Peter] Univ Calif Berkeley, Dept Astron, Berkeley, CA 94720 USA. [Cao, Yi; Kasliwal, Mansi] CALTECH, Dept Astron, Pasadena, CA 91125 USA. [Kasliwal, Mansi] Carnegie Inst Sci, Observ, Pasadena, CA 91101 USA. RP Nugent, P (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Computat Cosmol Ctr, 1 Cyclotron Rd, Berkeley, CA 94720 USA. EM penugent@LBL.gov NR 9 TC 0 Z9 0 U1 0 U2 1 PU SPIE-INT SOC OPTICAL ENGINEERING PI BELLINGHAM PA 1000 20TH ST, PO BOX 10, BELLINGHAM, WA 98227-0010 USA SN 0277-786X BN 978-1-62841-487-5 J9 PROC SPIE PY 2015 VL 9397 AR 939702 DI 10.1117/12.2085383 PG 7 WC Computer Science, Theory & Methods; Engineering, Electrical & Electronic; Optics SC Computer Science; Engineering; Optics GA BC1NC UT WOS:000350276200002 ER PT J AU Billinge, SJL Miao, JW AF Billinge, Simon J. L. Miao, Jianwei TI Celebrating the past, looking to the future SO ACTA CRYSTALLOGRAPHICA A-FOUNDATION AND ADVANCES LA English DT Editorial Material C1 [Billinge, Simon J. L.] Columbia Univ, Dept Appl Phys & Appl Math, New York, NY 10027 USA. [Billinge, Simon J. L.] Brookhaven Natl Lab, Condensed Matter Phys & Mat Sci Dept, Upton, NY 11973 USA. [Miao, Jianwei] Univ Calif Los Angeles, Dept Phys & Astron, Los Angeles, CA 90095 USA. [Miao, Jianwei] Univ Calif Los Angeles, Calif NanoSyst Inst, Los Angeles, CA 90095 USA. RP Billinge, SJL (reprint author), Columbia Univ, Dept Appl Phys & Appl Math, 200 Mudd,500 W 120th St, New York, NY 10027 USA. NR 1 TC 4 Z9 4 U1 2 U2 9 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0108-7673 EI 1600-5724 J9 ACTA CRYSTALLOGR A JI Acta Crystallogr. Sect. A PD JAN PY 2015 VL 71 BP 1 EP 2 DI 10.1107/S2053273314027685 PN 1 PG 2 WC Chemistry, Multidisciplinary; Crystallography SC Chemistry; Crystallography GA CC7KB UT WOS:000350545100001 PM 25537382 ER PT J AU Ramadhar, TR Zheng, SL Chen, YS Clardy, J AF Ramadhar, Timothy R. Zheng, Shao-Liang Chen, Yu-Sheng Clardy, Jon TI Analysis of rapidly synthesized guest-filled porous complexes with synchrotron radiation: practical guidelines for the crystalline sponge method SO ACTA CRYSTALLOGRAPHICA A-FOUNDATION AND ADVANCES LA English DT Article ID X-RAY-STRUCTURE; SINGLE-CRYSTAL; SUPRAMOLECULAR SOLIDS; 1,3-DIMETHYLCYCLOBUTADIENE; CONFINEMENT; MATRIX; CRYSTALLOGRAPHY AB A detailed set of synthetic and crystallographic guidelines for the crystalline sponge method based upon the analysis of expediently synthesized crystal sponges using third-generation synchrotron radiation are reported. The procedure for the synthesis of the zinc-based metal-organic framework used in initial crystal sponge reports has been modified to yield competent crystals in 3 days instead of 2 weeks. These crystal sponges were tested on some small molecules, with two being unexpectedly difficult cases for analysis with in-house diffractometers in regard to data quality and proper space-group determination. These issues were easily resolved by the use of synchrotron radiation using data-collection times of less than an hour. One of these guests induced a single-crystal-to-single-crystal transformation to create a larger unit cell with over 500 non-H atoms in the asymmetric unit. This led to a non-trivial refinement scenario that afforded the best Flack x absolute stereochemical determination parameter to date for these systems. The structures did not require the use of PLATON/SQUEEZE or other solvent-masking programs, and are the highest-quality crystalline sponge systems reported to date where the results are strongly supported by the data. A set of guidelines for the entire crystallographic process were developed through these studies. In particular, the refinement guidelines include strategies to refine the host framework, locate guests and determine occupancies, discussion of the proper use of geometric and anisotropic displacement parameter restraints and constraints, and whether to perform solvent squeezing/masking. The single-crystal-to-single-crystal transformation process for the crystal sponges is also discussed. The presented general guidelines will be invaluable for researchers interested in using the crystalline sponge method at in-house diffraction or synchrotron facilities, will facilitate the collection and analysis of reliable high-quality data, and will allow construction of chemically and physically sensible models for guest structural determination. C1 [Ramadhar, Timothy R.; Clardy, Jon] Harvard Univ, Sch Med, Dept Biol Chem & Mol Pharmacol, Boston, MA 02115 USA. [Zheng, Shao-Liang] Harvard Univ, Dept Chem & Chem Biol, Cambridge, MA 02138 USA. [Chen, Yu-Sheng] Univ Chicago, Adv Photon Source, ChemMatCARS, Ctr Adv Radiat Sources,Argonne Natl Lab, Argonne, IL 60439 USA. RP Clardy, J (reprint author), Harvard Univ, Sch Med, Dept Biol Chem & Mol Pharmacol, 240 Longwood Ave, Boston, MA 02115 USA. EM jon_clardy@hms.harvard.edu OI Ramadhar, Timothy/0000-0002-7063-5445 FU National Institutes of Health [R01-GM086258, U19-AI109673, F32-GM108415]; Divisions of Chemistry (CHE) and Materials Research (DMR), National Science Foundation [NSF/CHE-1346572]; US DOE [DE-AC02-06CH11357] FX We are grateful for financial support through the National Institutes of Health (R01-GM086258 and U19-AI109673 to JC and F32-GM108415 to TRR). ChemMatCARS Sector 15 is principally supported by the Divisions of Chemistry (CHE) and Materials Research (DMR), National Science Foundation, under grant No. NSF/CHE-1346572. Use of the Advanced Photon Source, an Office of Science User Facility operated for the US Department of Energy (DOE) Office of Science by Argonne National Laboratory, was supported by the US DOE under Contract No. DE-AC02-06CH11357. We thank Dr Christine Beemelmanns for preliminary studies on the synthesis of the MOF complexes. Finally, we thank both reviewers for their helpful insights and discussion during the peer-review process for this manuscript. NR 43 TC 22 Z9 22 U1 3 U2 32 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 0108-7673 EI 1600-5724 J9 ACTA CRYSTALLOGR A JI Acta Crystallogr. Sect. A PD JAN PY 2015 VL 71 BP 46 EP 58 DI 10.1107/S2053273314019573 PN 1 PG 13 WC Chemistry, Multidisciplinary; Crystallography SC Chemistry; Crystallography GA CC7KB UT WOS:000350545100007 PM 25537388 ER PT J AU Grzonka, D Kilian, K Ritman, J Sefzick, T Oelert, W Diermaier, M Widmann, E Zmeskal, J Glowacz, B Moskal, P Zielinski, M Wolke, M Nadel-Turonski, P Carmignotto, M Horn, T Mkrtchyan, H Asaturyan, A Mkrtchyan, A Tadevosyan, V Zhamkochyan, S Malbrunot-Ettenauer, S Eyrich, W Hauenstein, F Zink, A AF Grzonka, D. Kilian, K. Ritman, J. Sefzick, T. Oelert, W. Diermaier, M. Widmann, E. Zmeskal, J. Glowacz, B. Moskal, P. Zielinski, M. Wolke, M. Nadel-Turonski, P. Carmignotto, M. Horn, T. Mkrtchyan, H. Asaturyan, A. Mkrtchyan, A. Tadevosyan, V. Zhamkochyan, S. Malbrunot-Ettenauer, S. Eyrich, W. Hauenstein, F. Zink, A. TI SEARCH FOR POLARIZATION EFFECTS IN THE ANTIPROTON PRODUCTION PROCESS SO ACTA PHYSICA POLONICA B LA English DT Article ID COULOMB-NUCLEAR INTERFERENCE; PP ELASTIC-SCATTERING; P(P)OVER-BAR INTERACTION; PROTON; BEAMS; REGION; GEV/C; FACILITY AB For the production of a polarized antiproton beam, various methods have been suggested including the possibility that antiprotons may be produced polarized which will be checked experimentally. The polarization of antiprotons produced under typical conditions for antiproton beam preparation will be measured at the CERN/PS. If the production process creates some polarization, a polarized antiproton beam could be prepared by a rather simple modification of the antiproton beam facility. The detection setup and the expected experimental conditions are described. C1 [Grzonka, D.; Kilian, K.; Ritman, J.; Sefzick, T.] Forschungszentrum Julich, Inst Kernphys, D-52425 Julich, Germany. [Oelert, W.] Johannes Gutenberg Univ Mainz, D-55099 Mainz, Germany. [Diermaier, M.; Widmann, E.; Zmeskal, J.] Stefan Meyer Inst Subatomare Phys, A-1090 Vienna, Austria. [Glowacz, B.; Moskal, P.; Zielinski, M.] Jagiellonian Univ, Inst Phys, PL-30348 Krakow, Poland. [Wolke, M.] Uppsala Univ, Dept Phys & Astron, S-75120 Uppsala, Sweden. [Nadel-Turonski, P.] Thomas Jefferson Natl Accelerator Facil, Newport News, VA 23606 USA. [Carmignotto, M.; Horn, T.] Catholic Univ Amer, Dept Phys, Washington, DC 20064 USA. [Mkrtchyan, H.; Asaturyan, A.; Mkrtchyan, A.; Tadevosyan, V.; Zhamkochyan, S.] AI Alikhanyan Sci Lab, Yerevan 0036, Armenia. [Malbrunot-Ettenauer, S.] CERN, Dept Phys, CH-1211 Genve 23, Switzerland. [Eyrich, W.; Hauenstein, F.; Zink, A.] Univ Erlangen Nurnberg, D-91058 Erlangen, Germany. RP Grzonka, D (reprint author), Forschungszentrum Julich, Inst Kernphys, D-52425 Julich, Germany. RI Widmann, Eberhard/G-2545-2011; Zielinski, Marcin/B-6768-2014; Moskal, Pawel/S-9151-2016 OI Widmann, Eberhard/0000-0003-0486-6023; Zielinski, Marcin/0000-0002-9540-9911; Moskal, Pawel/0000-0002-4229-3548 FU Polish National Science Centre [2011/03/N/ST2/02653]; Polish Ministry of Science and Higher Education [393/E-338/STYP/8/2013]; DAAD Exchange Programme (PPP-Polen) FX This work was supported partially by the Polish National Science Centre through the Grant No. 2011/03/N/ST2/02653, and by the Polish Ministry of Science and Higher Education through grant No. 393/E-338/STYP/8/2013, and by DAAD Exchange Programme 2015 (PPP-Polen). NR 33 TC 1 Z9 1 U1 0 U2 0 PU WYDAWNICTWO UNIWERSYTETU JAGIELLONSKIEGO PI KRAKOW PA UL GRODZKA 26, KRAKOW, 31044, POLAND SN 0587-4254 EI 1509-5770 J9 ACTA PHYS POL B JI Acta Phys. Pol. B PD JAN PY 2015 VL 46 IS 1 BP 191 EP 201 DI 10.5506/APhysPolB.46.191 PG 11 WC Physics, Multidisciplinary SC Physics GA CC5QR UT WOS:000350416900025 ER PT J AU Damin, CA Nguyen, VHT Niyibizi, AS Smith, EA AF Damin, Craig A. Nguyen, Vy H. T. Niyibizi, Auguste S. Smith, Emily A. TI Application of scanning angle Raman spectroscopy for determining the location of buried polymer interfaces with tens of nanometer precision SO ANALYST LA English DT Article ID TOTAL INTERNAL-REFLECTION; HOMOGENEOUS MOLECULAR PROFILES; OPTICAL WAVE-GUIDES; THIN-FILM; DEPTH RESOLUTION; INTEGRATED-OPTICS; MICROSCOPY; SCATTERING; INTERFEROMETRY; THICKNESS AB Near-infrared scanning angle (SA) Raman spectroscopy was utilized to determine the interface location in bilayer films (a stack of two polymer layers) of polystyrene (PS) and polycarbonate (PC). Finite-difference-time- domain (FDTD) calculations of the sum square electric field (SSEF) for films with total bilayer thicknesses of 1200-3600 nm were used to construct models for simultaneously measuring the film thickness and the location of the buried interface between the PS and PC layers. Samples with total thicknesses of 1320, 1890, 2300, and 2750 nm and varying PS/PC interface locations were analyzed using SA Raman spectroscopy. Comparing SA Raman spectroscopy and optical profilometry measurements, the average percent difference in the total bilayer thickness was 2.0% for films less than similar to 2300 nm thick. The average percent difference in the thickness of the PS layer, which reflects the interface location, was 2.5% when the PS layer was less than similar to 1800 nm. SA Raman spectroscopy has been shown to be a viable, non-destructive method capable of determining the total bilayer thickness and buried interface location for bilayer samples consisting of thin polymer films with comparable indices of refraction. C1 [Damin, Craig A.; Nguyen, Vy H. T.; Niyibizi, Auguste S.; Smith, Emily A.] US DOE, Ames Lab, Ames, IA 50011 USA. [Damin, Craig A.; Nguyen, Vy H. T.; Smith, Emily A.] Iowa State Univ, Dept Chem, Ames, IA 50011 USA. RP Smith, EA (reprint author), US DOE, Ames Lab, Ames, IA 50011 USA. EM esmith1@iastate.edu OI Smith, Emily/0000-0001-7438-7808 FU U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences through Ames Laboratory; U.S. Department of Energy by Iowa State University [DE-AC02-07CH11358] FX This research is supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences through Ames Laboratory. The Ames Laboratory is operated for the U.S. Department of Energy by Iowa State University under Contract No. DE-AC02-07CH11358. The authors thank Wyman Martinek for his assistance with the optical profilometry measurements. NR 50 TC 1 Z9 1 U1 0 U2 9 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 0003-2654 EI 1364-5528 J9 ANALYST JI Analyst PY 2015 VL 140 IS 6 BP 1955 EP 1964 DI 10.1039/c4an02240h PG 10 WC Chemistry, Analytical SC Chemistry GA CC7UH UT WOS:000350573400029 PM 25669718 ER PT J AU Hasegawa, H Sonnerup, BUO Eriksson, S Nakamura, TKM Kawano, H AF Hasegawa, H. Sonnerup, B. U. Oe. Eriksson, S. Nakamura, T. K. M. Kawano, H. TI Dual-spacecraft reconstruction of a three-dimensional magnetic flux rope at the Earth's magnetopause SO ANNALES GEOPHYSICAE LA English DT Article DE Magnetospheric physics; magnetopause cusp and boundary layers; space plasma physics; magnetic reconnection; instruments and techniques ID LATITUDE BOUNDARY-LAYER; CLUSTER OBSERVATIONS; TRANSFER EVENTS; FIELD TOPOLOGY; NULL POINTS; SOLAR-WIND; X-LINE; RECONNECTION; PLASMA; MAGNETOMETER AB We present the first results of a data analysis method, developed by Sonnerup and Hasegawa (2011), for reconstructing three-dimensional (3-D), magnetohydrostatic structures from data taken as two closely spaced satellites traverse the structures. The method is applied to a magnetic flux transfer event (FTE), which was encountered on 27 June 2007 by at least three (TH-C, TH-D, and TH-E) of the five THEMIS probes near the subsolar magnetopause. The FTE was sandwiched between two oppositely directed reconnection jets under a southward interplanetary magnetic field condition, consistent with its generation by multiple X-line reconnection. The recovered 3-D field indicates that a magnetic flux rope with a diameter of similar to 3000 km was embedded in the magnetopause. The FTE flux rope had a significant 3-D structure, because the 3-D field reconstructed from the data from TH-C and TH-D (separated by similar to 390 km) better predicts magnetic field variations actually measured along the TH-E path than does the 2-D Grad-Shafranov reconstruction using the data from TH-C (which was closer to TH-E than TH-D and was at similar to 1250 km from TH-E). Such a 3D nature suggests that the field lines reconnected at the two X-lines on both sides of the flux rope are entangled in a complicated way through their interaction with each other. The generation process of the observed 3-D flux rope is discussed on the basis of the reconstruction results and the pitch-angle distribution of electrons observed in and around the FTE. C1 [Hasegawa, H.] Japan Aerosp Explorat Agcy, Inst Space & Astronaut Sci, Sagamihara, Kanagawa 2298510, Japan. [Sonnerup, B. U. Oe.] Dartmouth Coll, Thayer Sch Engn, Hanover, NH 03755 USA. [Eriksson, S.] Univ Colorado, Atmospher & Space Phys Lab, Boulder, CO 80309 USA. [Nakamura, T. K. M.] Los Alamos Natl Lab, Computat Phys Div X, Los Alamos, NM USA. [Kawano, H.] Kyushu Univ, Int Ctr Space Weather Sci & Educ, Fukuoka 812, Japan. RP Hasegawa, H (reprint author), Japan Aerosp Explorat Agcy, Inst Space & Astronaut Sci, 3-1-1 Yoshinodai, Sagamihara, Kanagawa 2298510, Japan. EM hase@stp.isas.jaxa.jp RI Hasegawa, Hiroshi/A-1192-2007; OI Hasegawa, Hiroshi/0000-0002-1172-021X; Eriksson, Stefan/0000-0002-5619-1577 FU JSPS [24740337]; NASA [NNX14AC38G] FX The authors thank the THEMIS team for successful management and operation of the mission and for allowing our use of the data from the ESA and FGM instruments. Work by H. Hasegawa at JAXA was supported by JSPS Grant-in-Aid for Scientific Research KAKENHI grant no. 24740337. Work at Dartmouth College was partially supported by NASA grant NNX14AC38G. NR 65 TC 3 Z9 3 U1 2 U2 9 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 0992-7689 EI 1432-0576 J9 ANN GEOPHYS-GERMANY JI Ann. Geophys. PY 2015 VL 33 IS 2 BP 169 EP 184 DI 10.5194/angeo-33-169-2015 PG 16 WC Astronomy & Astrophysics; Geosciences, Multidisciplinary; Meteorology & Atmospheric Sciences SC Astronomy & Astrophysics; Geology; Meteorology & Atmospheric Sciences GA CC7OY UT WOS:000350559000002 ER PT J AU Warren, JM Jensen, AM Medlyn, BE Norby, RJ Tissue, DT AF Warren, Jeffrey M. Jensen, Anna M. Medlyn, Belinda E. Norby, Richard J. Tissue, David T. TI Carbon dioxide stimulation of photosynthesis in Liquidambar styraciflua is not sustained during a 12-year field experiment SO AOB PLANTS LA English DT Article DE Acclimation; down-regulation; free-air CO2 enrichment; nitrogen limitation; sweetgum ID AIR CO2 ENRICHMENT; ELEVATED ATMOSPHERIC CO2; PROGRESSIVE NITROGEN LIMITATION; PINUS-TAEDA; TEMPERATE FOREST; LOBLOLLY-PINE; STOMATAL CONDUCTANCE; USE EFFICIENCY; LEAF PHOTOSYNTHESIS; DECIDUOUS FOREST AB Elevated atmospheric CO2 (eCO(2)) often increases photosynthetic CO2 assimilation (A) in field studies of temperate tree species. However, there is evidence that A may decline through time due to biochemical and morphological acclimation, and environmental constraints. Indeed, at the free-air CO2 enrichment (FACE) study in Oak Ridge, Tennessee, A was increased in 12-year-old sweetgum trees following 2 years of similar to 40 % enhancement of CO2. A was re-assessed a decade later to determine if the initial enhancement of photosynthesis by eCO(2) was sustained through time. Measurements were conducted at prevailing CO2 and temperature on detached, re-hydrated branches using a portable gas exchange system. Photosynthetic CO2 response curves (A versus the CO2 concentration in the intercellular air space (Ci); or A-Ci curves) were contrasted with earlier measurements using leaf photosynthesis model equations. Relationships between light-saturated photosynthesis (Asat), maximum electron transport rate (Jmax), maximum Rubisco activity (Vcmax), chlorophyll content and foliar nitrogen (N) were assessed. In 1999, Asat for eCO(2) treatmentswas 15.4+ 0.8 mmol m 22 s 21, 22 % higher than aCO(2) treatments (P, 0.01). By 2009, Asat declined to,50 % of 1999 values, and there was no longer a significant effect of eCO(2) (Asat similar to 6.9 or 5.7+ 0.7 mmol m 22 s 21 for eCO(2) or aCO(2), respectively). In 1999, there was no treatment effect on area-based foliar N; however, by 2008, N content in eCO(2) foliage was 17 % less than that in aCO(2) foliage. Photosynthetic N-use efficiency (Asat : N) was greater in eCO(2) in 1999 resulting in greater Asat despite similar N content, but the enhanced efficiency in eCO(2) trees was lost as foliar N declined to sub-optimal levels. There was no treatment difference in the declining linear relationships between Jmax or Vcmax with declining N, or in the ratio of Jmax : Vcmax through time. Results suggest that the initial enhancement of photosynthesis to elevated CO2 will not be sustained through time if N becomes limited. C1 [Warren, Jeffrey M.; Jensen, Anna M.; Norby, Richard J.] Oak Ridge Natl Lab, Climate Change Sci Inst, Oak Ridge, TN 37831 USA. [Warren, Jeffrey M.; Jensen, Anna M.; Norby, Richard J.] Oak Ridge Natl Lab, Div Environm Sci, Oak Ridge, TN 37831 USA. [Medlyn, Belinda E.] Macquarie Univ, Sch Biol Sci, Sydney, NSW 2019, Australia. [Tissue, David T.] Univ Western Sydney, Hawkesbury Inst Environm, Richmond, NSW 2753, Australia. RP Warren, JM (reprint author), Oak Ridge Natl Lab, Climate Change Sci Inst, Oak Ridge, TN 37831 USA. EM warrenjm@ornl.gov RI Warren, Jeffrey/B-9375-2012; Norby, Richard/C-1773-2012 OI Warren, Jeffrey/0000-0002-0680-4697; Norby, Richard/0000-0002-0238-9828 FU UT-Battelle, LLC [DE-AC05-00OR22725]; US Department of Energy FX The authors appreciate fieldwork and facility maintenance from Joanne Childs (arbornaut), Cassandra Bruno, Jeff Riggs and Danny Sluss, and data from Colleen Iversen and Carla Gunderson. This manuscript has been authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the US Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a nonexclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan). NR 76 TC 7 Z9 8 U1 13 U2 54 PU OXFORD UNIV PRESS PI OXFORD PA GREAT CLARENDON ST, OXFORD OX2 6DP, ENGLAND SN 2041-2851 J9 AOB PLANTS JI Aob Plants PY 2015 VL 7 AR plu074 DI 10.1093/aobpla/plu074 PG 13 WC Plant Sciences SC Plant Sciences GA CC7OT UT WOS:000350558500001 ER PT J AU Anderson-Cook, CM AF Anderson-Cook, Christine M. TI Opportunities to empower statisticians in emerging areas SO APPLIED STOCHASTIC MODELS IN BUSINESS AND INDUSTRY LA English DT Article DE Statistical engineering; meta-analysis; multiple data sources; resource allocation; decision making ID COMPLEX-SYSTEMS; RELIABILITY; OPTIMIZATION; CALIBRATION AB Statistics has long played an important role in impacting the practices of business and industry. As data collection strategies become more automated and first-principles scientific modeling with computer codes becomes more sophisticated, statistics has the opportunity to evolve and further contribute to the bottom line. Thinking about statistics as a set of tools to be applied piecemeal to a complex problem can be limiting. The emerging discussion about statistical engineering (as proposed by Roger Hoerl and Ronald Snee in Quality Progress, 2010) provides a framework for formalizing the role of statistics in a broader set of applications. Expanding how we think about data collection through resource allocation with multiple possible data types; combining data with first principles models of underlying science and engineering phenomena; and focusing on the multiple facets of the decision-making processall represent opportunities to expand the impact and influence of statistics. Statisticians have the opportunity to embrace these new opportunities to expand our sphere of influence and make broader contributions. Examples from collaborative efforts with subject matter experts at Los Alamos National Laboratory are presented to illustrate these emerging areas. Copyright (c) 2014 John Wiley & Sons, Ltd. C1 Los Alamos Natl Lab, Stat Sci Grp, Los Alamos, NM 87545 USA. RP Anderson-Cook, CM (reprint author), Los Alamos Natl Lab, Stat Sci Grp, Los Alamos, NM 87545 USA. EM c-and-cook@lanl.gov NR 34 TC 1 Z9 1 U1 0 U2 4 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 1524-1904 EI 1526-4025 J9 APPL STOCH MODEL BUS JI Appl. Stoch. Models. Bus. Ind. PD JAN-FEB PY 2015 VL 31 IS 1 SI SI BP 3 EP 11 DI 10.1002/asmb.2067 PG 9 WC Operations Research & Management Science; Mathematics, Interdisciplinary Applications; Statistics & Probability SC Operations Research & Management Science; Mathematics GA CC6BX UT WOS:000350450700002 ER PT J AU Anderson-Cook, CM AF Anderson-Cook, Christine M. TI Rejoinder to 'Opportunities to empower statisticians in emerging areas' SO APPLIED STOCHASTIC MODELS IN BUSINESS AND INDUSTRY LA English DT Editorial Material DE statistical engineering; meta-analysis; multiple data sources C1 Los Alamos Natl Lab, Los Alamos, NM 87545 USA. RP Anderson-Cook, CM (reprint author), Los Alamos Natl Lab, Los Alamos, NM 87545 USA. EM c-and-cook@lanl.gov NR 0 TC 0 Z9 0 U1 0 U2 1 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 1524-1904 EI 1526-4025 J9 APPL STOCH MODEL BUS JI Appl. Stoch. Models. Bus. Ind. PD JAN-FEB PY 2015 VL 31 IS 1 SI SI BP 15 EP 15 DI 10.1002/asmb.2070 PG 1 WC Operations Research & Management Science; Mathematics, Interdisciplinary Applications; Statistics & Probability SC Operations Research & Management Science; Mathematics GA CC6BX UT WOS:000350450700004 ER PT J AU Chu, HH Yen, CW Hayden, SC AF Chu, Hunghao Yen, Chun-Wan Hayden, Steven C. TI Fabrication of Biosensing Surfaces Using Adhesive Polydopamine SO BIOTECHNOLOGY PROGRESS LA English DT Article DE biosensing; functional surface coating; SERS; polydopamine; gold nanoparticles ID MUSSEL-INSPIRED POLYDOPAMINE; MULTIFUNCTIONAL COATINGS; GOLD NANOPARTICLES; VERSATILE PLATFORM; GRAPHENE SHEETS; DOPAMINE; SCAFFOLD; POLYMERIZATION; HYBRID AB Dopamine can be induced to polymerize on a variety of substrates, providing a robust and bioinspired surface coating that can be used to tune substrate surface properties and to sequester other species at the interface. We first exploit the facile nature of this surface modification procedure to generate an array of polydopamine that, in conjunction with fluorescent tags, provides the ability to detect multiple protein targets simultaneously and with great specificity. We then demonstrate the use of polydopamine as a matrix to confine gold nanoparticles at the surface of glass and graphene substrates. The nanoparticles (NPs) are used to template further gold nanoparticle growth in situ at the interface; subsequent calcination to remove the polydopamine matrix and sinter the NPs generates a highly active surface enhanced Raman scattering surface that allows for sensitive molecular detection. These varied uses in surface modification/biosensing demonstrate the utility of polydopamine as a functional surface modification for control of physical and electronic properties at the interface. (c) 2014 American Institute of Chemical Engineers Biotechnol. Prog., 31:299-306, 2015 C1 [Chu, Hunghao] Childrens Hosp, Dept Anesthesiol, Boston, MA 02115 USA. [Chu, Hunghao] MIT, Koch Inst Integrat Canc Res, Cambridge, MA 02139 USA. [Yen, Chun-Wan] MIT, Inst Med Engn & Sci, Cambridge, MA 02139 USA. [Hayden, Steven C.] Los Alamos Natl Lab, Mat Phys & Applicat Div, Los Alamos, NM 87545 USA. RP Chu, HH (reprint author), Childrens Hosp, Dept Anesthesiol, 300 Longwood Ave, Boston, MA 02115 USA. EM hunghao.chu@childrens.harvard.edu NR 38 TC 2 Z9 2 U1 8 U2 77 PU WILEY-BLACKWELL PI HOBOKEN PA 111 RIVER ST, HOBOKEN 07030-5774, NJ USA SN 8756-7938 EI 1520-6033 J9 BIOTECHNOL PROGR JI Biotechnol. Prog. PD JAN-FEB PY 2015 VL 31 IS 1 BP 299 EP 306 DI 10.1002/btpr.1991 PG 8 WC Biotechnology & Applied Microbiology; Food Science & Technology SC Biotechnology & Applied Microbiology; Food Science & Technology GA CC3KR UT WOS:000350247900034 PM 25219782 ER PT J AU Kuhl, AL AF Kuhl, A. L. TI On the structure of self-similar detonation waves in TNT charges SO COMBUSTION EXPLOSION AND SHOCK WAVES LA English DT Article DE detonation waves in TNT; phase-plane method; similarity solution; CJ conditions; species concentrations ID SIMILAR BLAST WAVES AB A phase-plane method is proposed to model flow fields bounded by constant-velocity detonation waves propagating in TNT charges. Similarity transformations are used to formulate the problem in the phase plane of non-dimensional sound speed Z versus non-dimensional velocity F. The formulation results in two coupled ordinary differential equations that are solved simultaneously. The solution corresponds to an integral curve Z(F) in the phase plane, starting at the Chapman-Jouguet (CJ) point and terminating at the singularity A, which is the sonic point within the wave. The system is closed by computing thermodynamic variables along the expansion isentrope passing through the CJ point, forming, in effect, the complete equation of state of the thermodynamic system. The CJ condition and isentropic states are computed by the Cheetah thermodynamic code. Solutions are developed for planar, cylindrical, and spherical detonations. Species profiles are also computed; carbon graphite is found to be the predominant component (a parts per thousand 10 mol/kg). The similarity solution is used to initialize a 1D gas-dynamic simulation that predicts the initial expansion of the detonation products and the formation of a blast wave in air. Such simulations provide an insight into the thermodynamic states and species concentrations that create the initial optical emissions from TNT fireballs. C1 Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. RP Kuhl, AL (reprint author), Lawrence Livermore Natl Lab, Livermore, CA 94550 USA. EM kuhl2@llnl.gov FU U.S. Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07NA27344]; Department of Homeland Security ST [HSHQPM-10-X-00070] FX This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory (Contract No. DE-AC52-07NA27344) and the Department of Homeland Security S&T (Contract No. HSHQPM-10-X-00070). Their support is gratefully appreciated. NR 18 TC 0 Z9 0 U1 4 U2 7 PU MAIK NAUKA/INTERPERIODICA/SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013-1578 USA SN 0010-5082 EI 1573-8345 J9 COMBUST EXPLO SHOCK+ JI Combust. Explos. PD JAN PY 2015 VL 51 IS 1 BP 72 EP 79 DI 10.1134/S0010508215010074 PG 8 WC Thermodynamics; Energy & Fuels; Engineering, Multidisciplinary; Engineering, Chemical; Materials Science, Multidisciplinary SC Thermodynamics; Energy & Fuels; Engineering; Materials Science GA CC4VW UT WOS:000350353700007 ER PT J AU Giannopoulos, DP Wilson-Konderka, C Gagnon, KJ Teat, SJ Escuer, A Metallinos, C Stamatatos, TC AF Giannopoulos, Dimosthenis P. Wilson-Konderka, Cody Gagnon, Kevin J. Teat, Simon J. Escuer, Albert Metallinos, Costa Stamatatos, Theocharis C. TI Synthesis and first use of pyridine-2,6-diylbis(pyrazine-2-ylmethanone) in metal cluster chemistry: a {(Mn3Na2)-Na-III} complex with an ideal trigonal bipyramidal geometry SO DALTON TRANSACTIONS LA English DT Article ID SINGLE-MOLECULE MAGNETS; OXYGEN-EVOLVING COMPLEX; CENTERED MANGANESE COMPLEXES; HIGH-SPIN MOLECULES; CRYSTAL-STRUCTURES; DI-2-PYRIDYL KETONE; HIGH-NUCLEARITY; PHOTOSYSTEM-II; CHAIN MAGNET; CU-II AB The successful organic synthesis of a new dipyrazole/pyridine-dicarbonyl organic molecule, namely pyridine-2,6-diylbis(pyrazine-2-ylmethanone) [(pz)CO(py)CO(pz)], followed by its employment in Mn coordination chemistry has yielded the neutral cluster compound [Mn3Na2O(N-3)(3)(L)(3)] (1), where L2- is the (pz) C-(CH2COCH3)(O-)(py)C(CH2COCH3)(O-)(pz)dianion. The latter group was formed in situ, presumably by the nucleophilic attack of the carbanion -CH2COCH3 to the carbonyl carbon atoms of (pz) CO(py) CO( pz), in the presence of Mnn+ ions under basic conditions and in solvent Me2CO. Complex 1 possesses an almost ideal trigonal bipyramidal topology, with the two Na+ ions occupying the apical positions and the three Mn-III ions residing in the equatorial trigonal plane. The bridging ligation about the metal ions is provided by a mu(3)-O-2-ion and six mu-OR-groups from the L-2-ligand, while peripheral ligation is completed by three terminal azido groups and the pyridine N and carbonyl O atoms of L2-. Magnetic susceptibility studies revealed the presence of predominant antiferromagnetic exchange interactions between the paramagnetic Mn-III centres; the use of an anisotropic, equilateral Mn-3(III) triangle model allowed us to fit the magnetic data and obtain the best-fit parameters: J = -10.8 cm(-1), D = -5.3 cm(-1), and g = 1.99. The combined results demonstrate the rich chemical reactivity of carbonyl groups and the ability of poly-ketone ligands to stabilize cluster compounds with unprecedented structural motifs and interesting architectures. C1 [Giannopoulos, Dimosthenis P.; Wilson-Konderka, Cody; Metallinos, Costa; Stamatatos, Theocharis C.] Brock Univ, Dept Chem, St Catharines, ON L2S 3A1, Canada. [Gagnon, Kevin J.; Teat, Simon J.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA. [Escuer, Albert] Univ Barcelona, Dept Quim Inorgan, E-08028 Barcelona, Spain. RP Stamatatos, TC (reprint author), Brock Univ, Dept Chem, St Catharines, ON L2S 3A1, Canada. EM tstamatatos@brocku.ca RI Escuer, Albert/L-4706-2014 OI Escuer, Albert/0000-0002-6274-6866 FU Brock University; NSERC; CICYT [CTQ2009-07264]; Excellence in Research ICREA-Academia Award; Office of Science, Office of Basic Energy Sciences of the U.S. Department of Energy [DE-AC02-05CH11231] FX This work was supported by Brock University and NSERC Discovery Grant (Th.C.S and C.M), the CICYT (project CTQ2009-07264) and Excellence in Research ICREA-Academia Award (to A.E). The Advance 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. C.W.-K. would like to thank Prof. Tomas Hudlicky for assistance with the purification of L-2 and (pz)CO(py)CO(pz). NR 78 TC 0 Z9 0 U1 1 U2 18 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 1477-9226 EI 1477-9234 J9 DALTON T JI Dalton Trans. PY 2015 VL 44 IS 9 BP 4318 EP 4327 DI 10.1039/c4dt03666b PG 10 WC Chemistry, Inorganic & Nuclear SC Chemistry GA CB9ZI UT WOS:000349993400048 PM 25639266 ER PT J AU Reu, PL Sweatt, W Miller, T Fleming, D AF Reu, P. L. Sweatt, W. Miller, T. Fleming, D. TI Camera System Resolution and its Influence on Digital Image Correlation SO EXPERIMENTAL MECHANICS LA English DT Article DE Digital image correlation; Uncertainty quantification; Optical measurements; Full-field measurement; Lens resolution ID INTENSITY PATTERN NOISE; ERRORS; STRAIN; INTERPOLATION AB Digital image correlation (DIC) uses images from a camera and lens system to make quantitative measurements of the shape, displacement, and strain of test objects. This increasingly popular method has had little research on the influence of the imaging system resolution on the DIC results. This paper investigates the entire imaging system and studies how both the camera and lens resolution influence the DIC results as a function of the system Modulation Transfer Function (MTF). It will show that when making spatial resolution decisions (including speckle size) the resolution limiting component should be considered. A consequence of the loss of spatial resolution is that the DIC uncertainties will be increased. This is demonstrated using both synthetic and experimental images with varying resolution. The loss of image resolution and DIC accuracy can be compensated for by increasing the subset size, or better, by increasing the speckle size. The speckle-size and spatial resolution are now a function of the lens resolution rather than the more typical assumption of the pixel size. The paper will demonstrate the tradeoffs associated with limited lens resolution. C1 [Reu, P. L.; Sweatt, W.; Miller, T.; Fleming, D.] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Reu, PL (reprint author), Sandia Natl Labs, POB 5800, Albuquerque, NM 87185 USA. EM plreu@sandia.gov FU United States Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX Sandia is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the United States Department of Energy's National Nuclear Security Administration under contract No. DE-AC04-94AL85000. NR 19 TC 6 Z9 6 U1 3 U2 15 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 0014-4851 EI 1741-2765 J9 EXP MECH JI Exp. Mech. PD JAN PY 2015 VL 55 IS 1 SI SI BP 9 EP 25 DI 10.1007/s11340-014-9886-y PG 17 WC Materials Science, Multidisciplinary; Mechanics; Materials Science, Characterization & Testing SC Materials Science; Mechanics GA CC3LX UT WOS:000350251700002 ER PT J AU Lin, YZ Huang, LJ AF Lin, Youzuo Huang, Lianjie TI Acoustic- and elastic-waveform inversion using a modified total-variation regularization scheme SO GEOPHYSICAL JOURNAL INTERNATIONAL LA English DT Article DE Numerical solutions; Inverse theory; Numerical approximations and analysis; Non-linear differential equations; Body waves; Seismic tomography; Computational seismology ID IMAGE-RECONSTRUCTION; SEISMIC DATA; TIME; INFORMATION; RESTORATION; TOMOGRAPHY; ALGORITHMS AB Subsurface velocities within the Earth often contain piecewise-constant structures with sharp interfaces. Acoustic-and elastic-waveform inversion (AEWI) usually produces smoothed inversion results of subsurface geophysical properties. We develop novel AEWI methods using a modified total-variation regularization scheme to preserve sharp interfaces in piecewise-constant structures and improve the accuracy of compressional-and shear wave velocity inversion. We use an alternating-minimization algorithm to solve the minimization problem of our new waveform inversion methods. We decouple the original optimization problem into two simple subproblems: a standard waveform inversion subproblem with the Tikhonov regularization and a standard L-2-TV subproblem. We solve these two subproblems separately using the non-linear conjugate-gradient and split-Bregman iterative methods. The computational costs of our new waveform inversion methods using the modified total-variation regularization scheme are comparable to those of conventional waveform inversion approaches. Our numerical examples using synthetic seismic reflection data show that our new methods not only preserve sharp interfaces of subsurface structures, but also significantly improve the accuracy of compressional-and shear wave velocity inversion. C1 [Lin, Youzuo; Huang, Lianjie] Los Alamos Natl Lab, Geophys Grp, Los Alamos, NM 87545 USA. RP Lin, YZ (reprint author), Los Alamos Natl Lab, Geophys Grp, MS D452, Los Alamos, NM 87545 USA. EM ylin@lanl.gov FU U.S. Department of Energy [DE-AC52-06NA25396] FX This work was supported the U.S. Department of Energy through contract DE-AC52-06NA25396 to Los Alamos National Laboratory (LANL). The computation was performed on supercomputers provided by LANL's Institutional Computing Program. We thank Dr John Queen of Hi-Q Geophysical Inc. for providing us with a velocity model of the Brady's EGS field. We thank Antoine Guitton and an anonymous reviewer for their valuable comments. NR 40 TC 6 Z9 6 U1 1 U2 6 PU OXFORD UNIV PRESS PI OXFORD PA GREAT CLARENDON ST, OXFORD OX2 6DP, ENGLAND SN 0956-540X EI 1365-246X J9 GEOPHYS J INT JI Geophys. J. Int. PD JAN PY 2015 VL 200 IS 1 BP 489 EP 502 DI 10.1093/gji/ggu393 PG 14 WC Geochemistry & Geophysics SC Geochemistry & Geophysics GA CC0QU UT WOS:000350041600035 ER PT J AU Elliott, J Muller, C Deryng, D Chryssanthacopoulos, J Boote, KJ Buchner, M Foster, I Glotter, M Heinke, J Iizumi, T Izaurralde, RC Mueller, ND Ray, DK Rosenzweig, C Ruane, AC Sheffield, J AF Elliott, J. Mueller, C. Deryng, D. Chryssanthacopoulos, J. Boote, K. J. Buechner, M. Foster, I. Glotter, M. Heinke, J. Iizumi, T. Izaurralde, R. C. Mueller, N. D. Ray, D. K. Rosenzweig, C. Ruane, A. C. Sheffield, J. TI The Global Gridded Crop Model Intercomparison: data and modeling protocols for Phase 1 (v1.0) SO GEOSCIENTIFIC MODEL DEVELOPMENT LA English DT Article ID LAND-SURFACE MODEL; CLIMATE-CHANGE; SYSTEMS SIMULATION; HIGH-RESOLUTION; WATER; CARBON; YIELD; AGRICULTURE; PATTERNS; GROWTH AB We present protocols and input data for Phase 1 of the Global Gridded Crop Model Intercomparison, a project of the Agricultural Model Intercomparison and Improvement Project (AgMIP). The project includes global simulations of yields, phenologies, and many land-surface fluxes using 12-15 modeling groups for many crops, climate forcing data sets, and scenarios over the historical period from 1948 to 2012. The primary outcomes of the project include (1) a detailed comparison of the major differences and similarities among global models commonly used for large-scale climate impact assessment, (2) an evaluation of model and ensemble hindcasting skill, (3) quantification of key uncertainties from climate input data, model choice, and other sources, and (4) a multi-model analysis of the agricultural impacts of large-scale climate extremes from the historical record. C1 [Elliott, J.; Foster, I.] Univ Chicago, Chicago, IL 60637 USA. [Elliott, J.; Foster, I.] Argonne Natl Lab, Computat Inst, Chicago, IL USA. [Mueller, C.; Buechner, M.; Heinke, J.] Potsdam Inst Climate Impact Res, Potsdam, Germany. [Deryng, D.] Univ E Anglia, Tyndall Ctr, Norwich NR4 7TJ, Norfolk, England. [Chryssanthacopoulos, J.] Columbia Univ, Ctr Climate Syst Res, New York, NY USA. [Boote, K. J.] Univ Florida, Dept Agron, Gainesville, FL 32611 USA. [Glotter, M.] Univ Chicago, Dept Geophys Sci, Chicago, IL 60637 USA. [Heinke, J.] Int Livestock Res Inst, Nairobi, Kenya. [Iizumi, T.] Natl Inst Agroenvironm Sci, Tsukuba, Ibaraki 305, Japan. [Izaurralde, R. C.] Univ Maryland, Dept Geog Sci, College Pk, MD 20742 USA. [Mueller, N. D.] Harvard Univ, Ctr Environm, Cambridge, MA 02138 USA. [Ray, D. K.] Univ Minnesota, Inst Environm, St Paul, MN 55108 USA. [Rosenzweig, C.; Ruane, A. C.] NASA, Goddard Inst Space Studies, New York, NY 10025 USA. [Sheffield, J.] Princeton Univ, Dept Civil & Environm Engn, Princeton, NJ 08544 USA. [Heinke, J.] CSIRO, St Lucia, Qld 4067, Australia. RP Elliott, J (reprint author), Univ Chicago, Chicago, IL 60637 USA. EM jelliott@ci.uchicago.edu; cmueller@pik-potsdam.de RI Deryng, Delphine/F-7417-2010; Mueller, Christoph/E-4812-2016 OI Deryng, Delphine/0000-0001-6214-7241; Boote, Kenneth/0000-0002-1358-5496; Mueller, Christoph/0000-0002-9491-3550 FU National Science Foundation [SBE-0951576, GEO-1215910]; KULUNDA project [01LL0905L]; FACCE MACSUR project through the German Federal Ministry of Education and Research (BMBF) [031A103B] FX J. Elliott acknowledges financial support from the National Science Foundation under grants SBE-0951576 and GEO-1215910. C. Muller acknowledges financial support from the KULUNDA project (01LL0905L) and the FACCE MACSUR project (031A103B) funded through the German Federal Ministry of Education and Research (BMBF). Computing and data resources provided through the University of Chicago Research Computing Center. NR 58 TC 21 Z9 21 U1 5 U2 34 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 2015 VL 8 IS 2 BP 261 EP 277 DI 10.5194/gmd-8-261-2015 PG 17 WC Geosciences, Multidisciplinary SC Geology GA CC7OM UT WOS:000350557800008 ER PT J AU Berg, LK Shrivastava, M Easter, RC Fast, JD Chapman, EG Liu, Y Ferrare, RA AF Berg, L. K. Shrivastava, M. Easter, R. C. Fast, J. D. Chapman, E. G. Liu, Y. Ferrare, R. A. TI A new WRF-Chem treatment for studying regional-scale impacts of cloud processes on aerosol and trace gases in parameterized cumuli SO GEOSCIENTIFIC MODEL DEVELOPMENT LA English DT Article ID MODELING ORGANIC AEROSOLS; BASIS-SET APPROACH; CONVECTIVE PARAMETERIZATION; RADIATIVE IMPACT; CLIMATE SIMULATIONS; NUMERICAL-MODEL; BOUNDARY-LAYER; AIR-QUALITY; WEATHER; PRECIPITATION AB A new treatment of cloud effects on aerosol and trace gases within parameterized shallow and deep convection, and aerosol effects on cloud droplet number, has been implemented in the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) version 3.2.1 that can be used to better understand the aerosol life cycle over regional to synoptic scales. The modifications to the model include treatment of the cloud droplet number mixing ratio; key cloud microphysical and macrophysical parameters (including the updraft fractional area, updraft and downdraft mass fluxes, and entrainment) averaged over the population of shallow clouds, or a single deep convective cloud; and vertical transport, activation/resuspension, aqueous chemistry, and wet removal of aerosol and trace gases in warm clouds. These changes have been implemented in both the WRF-Chem chemistry packages as well as the Kain Fritsch (KF) cumulus parameterization that has been modified to better represent shallow convective clouds. Testing of the modified WRF-Chem has been completed using observations from the Cumulus Humilis Aerosol Processing Study (CHAPS). The simulation results are used to investigate the impact of cloud aerosol interactions on regional-scale transport of black carbon (BC), organic aerosol (OA), and sulfate aerosol. Based on the simulations presented here, changes in the columnintegrated BC can be as large as 50% when cloud aerosol interactions are considered (due largely to wet removal), or as large as +40 % for sulfate under non-precipitating conditions due to sulfate production in the parameterized clouds. The modifications to WRF-Chem are found to account for changes in the cloud droplet number concentration (CDNC) and changes in the chemical composition of cloud droplet residuals in a way that is consistent with observations collected during CHAPS. Efforts are currently underway to port the changes described here to the latest version of WRFChem, and it is anticipated that they will be included in a future public release of WRF-Chem. C1 [Berg, L. K.; Shrivastava, M.; Easter, R. C.; Fast, J. D.; Chapman, E. G.; Liu, Y.] Pacific NW Natl Lab, Richland, WA 99352 USA. [Ferrare, R. A.] NASA, Langley Res Ctr, Hampton, VA 23665 USA. RP Berg, LK (reprint author), Pacific NW Natl Lab, Richland, WA 99352 USA. EM larry.berg@pnnl.gov RI Berg, Larry/A-7468-2016 OI Berg, Larry/0000-0002-3362-9492 FU Office of Science of the US Department of Energy as part of the Atmospheric System Research (ASR) program; NASA Science Mission Directorate; Department of Energy ASR program; NASA CALIPSO project; [DE-AC06-76RLO 1830] FX This research was supported by the Office of Science of the US Department of Energy as part of the Atmospheric System Research (ASR) program. The Pacific Northwest National Laboratory is operated by Battelle Memorial Institute under contract DE-AC06-76RLO 1830. The funding for the B200 and HSRL operations came from the NASA Science Mission Directorate, the Department of Energy ASR program, and the NASA CALIPSO project. The authors would also like to thank the NASA Langley King Air B-200 and DOE G-1 flight crews for their outstanding work in supporting these flights and measurements. J. Ogren of NOAA and E. Andrews of the Cooperative Institute for Research in Environmental Sciences (CIRES) deployed the CVI during CHAPS. Data from the AMS were collected by Y.-N. Lee of Brookhaven National Laboratory (BNL), M. L. Alexander of the Pacific Northwest National Laboratory and J. Jayne of Aerodyne. Size distribution data were provided by G. Senum of BNL. G. Grell (NOAA) and R. Leung (PNNL) provided feedback on various aspects of the manuscript. We also thank three anonymous reviewers for valuable feedback on the manuscript. NR 80 TC 6 Z9 6 U1 1 U2 27 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 2015 VL 8 IS 2 BP 409 EP 429 DI 10.5194/gmd-8-409-2015 PG 21 WC Geosciences, Multidisciplinary SC Geology GA CC7OM UT WOS:000350557800015 ER PT J AU Tang, J Huang, YR Nguyen, DH Costes, SV Snijders, AM Mao, JH AF Tang, Jonathan Huang, Yurong Nguyen, David H. Costes, Sylvain V. Snijders, Antoine M. Mao, Jian-Hua TI Genetic Background Modulates lncRNA-Coordinated Tissue Response to Low Dose Ionizing Radiation SO INTERNATIONAL JOURNAL OF GENOMICS LA English DT Article ID ATOMIC-BOMB SURVIVORS; BREAST-CANCER RISK; NONCODING RNAS; CHILDHOOD; METASTASIS AB Long noncoding RNAs (lncRNAs) are emerging as key regulators of diverse cell functions and processes. However, the relevance of lncRNAs in the cell and tissue response to ionizing radiation has not yet been characterized. Here we used microarray profiling to determine lncRNA and mRNA expression in mammary glands of BALB/c and SPRET/EiJ mice after low-dose ionizing radiation (LDIR) exposure. We found that unirradiated mammary tissues of these strains differed significantly in baseline expressions of 290 lncRNAs. LDIR exposure (10 cGy) induced a significant change in the expression of many lncRNAs. The vast majority of lncRNAs identified to be differentially expressed after LDIR in either BALB/c or SPRET/EiJ had a significantly correlated expression pattern with at least one LDIR responsive mRNA. Functional analysis revealed that the response to LDIR in BALB/c mice is highly dynamic with enrichment for genes involved in tissue injury, inflammatory responses, and mammary gland development at 2, 4, and 8 weeks after LDIR, respectively. Our study demonstrates that genetic background strongly influences the expression of lncRNAs and their response to radiation and that lncRNAs may coordinate the tissue response to LDIR exposure via regulation of coding mRNAs. C1 [Tang, Jonathan; Huang, Yurong; Nguyen, David H.; Costes, Sylvain V.; Snijders, Antoine M.; Mao, Jian-Hua] Lawrence Berkeley Natl Lab, Div Life Sci, Berkeley, CA 94720 USA. RP Snijders, AM (reprint author), Lawrence Berkeley Natl Lab, Div Life Sci, 1 Cyclotron Rd MS977, Berkeley, CA 94720 USA. EM amsnijders@lbl.gov; jhmao@lbl.gov FU Office of Science, Office of Biological and Environmental Research, of the U.S. Department of Energy [DE-AC02-05CH11231] FX This work was supported by Low Dose SFA Program of the Director, Office of Science, Office of Biological and Environmental Research, of the U.S. Department of Energy under Contract no. DE-AC02-05CH11231. NR 22 TC 0 Z9 0 U1 2 U2 6 PU HINDAWI PUBLISHING CORP PI NEW YORK PA 410 PARK AVENUE, 15TH FLOOR, #287 PMB, NEW YORK, NY 10022 USA SN 2314-436X EI 2314-4378 J9 INT J GENOMICS JI Int. J. Genomics PY 2015 AR 461038 DI 10.1155/2015/461038 PG 7 WC Biochemistry & Molecular Biology; Biotechnology & Applied Microbiology; Genetics & Heredity SC Biochemistry & Molecular Biology; Biotechnology & Applied Microbiology; Genetics & Heredity GA CC4XY UT WOS:000350360700001 ER PT J AU Krishnan, PSSR Aguiar, JA Ramasse, QM Kepaptsoglou, DM Liang, WI Chu, YH Browning, ND Munroe, P Nagarajan, V AF Krishnan, P. S. Sankara Rama Aguiar, Jeffery A. Ramasse, Q. M. Kepaptsoglou, D. M. Liang, W. -I. Chu, Y. -H. Browning, N. D. Munroe, P. Nagarajan, V. TI Mapping strain modulated electronic structure perturbations in mixed phase bismuth ferrite thin films SO JOURNAL OF MATERIALS CHEMISTRY C LA English DT Article ID TRANSITION-METALS; OXIDATION-STATES; FINE-STRUCTURES; BIFEO3; SPECTROSCOPY; INTERFACES; POLARIZATION; MINERALS; OXIDES; FE AB Strain engineering of epitaxial ferroelectrics has emerged as a powerful method to tailor the electromechanical response of these materials, although the effect of strain at the atomic scale and the interplay between lattice displacements and electronic structure changes are not yet fully understood. Here, using a combination of scanning transmission electron microscopy (STEM) and density functional theory (DFT), we systematically probe the role of epitaxial strain in mixed phase bismuth ferrite thin films. Electron energy loss O K and Fe L-2,L-3 edge spectra acquired across the rhombohedral (R)-tetragonal (T) phase boundary reveal progressive, and systematic, changes in electronic structure going from one phase to the other. The comparison of the acquired spectra with theoretical simulations using DFT suggests a breakage in the structural symmetry across the boundary due to the simultaneous presence of increasing epitaxial strain and off-axial symmetry in the T phase. This implies that the imposed epitaxial strain plays a significant role in not only changing the crystal-field geometry, but also the bonding environment surrounding the central iron cation at the interface thus providing new insights and a possible link to understand how the imposed strain could perturb magnetic ordering in the T phase BFO. C1 [Krishnan, P. S. Sankara Rama; Munroe, P.; Nagarajan, V.] Univ New S Wales, Sch Mat Sci & Engn, Sydney, NSW 2052, Australia. [Aguiar, Jeffery A.] Los Alamos Natl Lab, Div Mat Sci & Technol, Los Alamos, NM 87545 USA. [Aguiar, Jeffery A.] Natl Renewable Energy Lab, Golden, CO 80401 USA. [Ramasse, Q. M.; Kepaptsoglou, D. M.] SuperSTEM Lab, Daresbury WA4 4AD, England. [Liang, W. -I.; Chu, Y. -H.] Natl Chiao Tung Univ, Dept Mat Sci & Engn, Hsinchu 30010, Taiwan. [Browning, N. D.] Pacific NW Natl Lab, Fundamental & Computat Sci Directorate, Richland, WA 99352 USA. RP Nagarajan, V (reprint author), Univ New S Wales, Sch Mat Sci & Engn, Sydney, NSW 2052, Australia. EM nagarajan@unsw.edu.au RI valanoor, nagarajan/B-4159-2012; Munroe, Paul/I-9313-2016; Ying-Hao, Chu/A-4204-2008; OI Munroe, Paul/0000-0002-5091-2513; Ying-Hao, Chu/0000-0002-3435-9084; Browning, Nigel/0000-0003-0491-251X; Aguiar, Jeffery/0000-0001-6101-4762 FU ARC; U. K. Engineering and Physical Sciences Research Council (EPSRC); Center for Materials at Irradiation and Mechanical Extremes (CMIME), an Energy Frontier Research Center - U. S. Department of Energy, Office of Science, Office of Basic Energy Sciences [2008LANL1026]; Chemical Imaging Initiative; Laboratory Directed Research and Development Program at Pacific Northwest National Laboratory (PNNL); U. S. Department of Energy (DOE) [DE-AC05-76RL01830] FX PSS thanks Adam Sikorski (ACMM, University of Sydney) for assistance provided during the cross-sectional specimen preparation. This work at The University of New South Wales was supported by an ARC Discovery project. The authors acknowledge access to the UNSW node of the Australian Microscopy & Microanalysis Research Facility (AMMRF). The SuperSTEM Laboratory is the U. K. National Facility for Aberration-Corrected Scanning Transmission Electron Microscopy, supported by the U. K. Engineering and Physical Sciences Research Council (EPSRC). Our sincere acknowledgement also goes to Prof. Nicola Spaldin and Dr Alison Hatt for generously sharing the structure files for the T' and R' phases. JAA acknowledges support from the Center for Materials at Irradiation and Mechanical Extremes (CMIME), an Energy Frontier Research Center funded by the U. S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Award Number 2008LANL1026 to utilize high performance computing facilities at Los Alamos National Laboratory. NB acknowledges support from by the Chemical Imaging Initiative; under the Laboratory Directed Research and Development Program at Pacific Northwest National Laboratory (PNNL), a multi-program national laboratory operated by Battelle for the U. S. Department of Energy (DOE) under Contract DE-AC05-76RL01830. NR 61 TC 6 Z9 6 U1 5 U2 46 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7526 EI 2050-7534 J9 J MATER CHEM C JI J. Mater. Chem. C PY 2015 VL 3 IS 8 BP 1835 EP 1845 DI 10.1039/c4tc02064b PG 11 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA CB6SZ UT WOS:000349758300029 ER PT J AU Bulaevskaya, V Wharton, S Clifton, A Qualley, G Miller, WO AF Bulaevskaya, V. Wharton, S. Clifton, A. Qualley, G. Miller, W. O. TI Wind power curve modeling in complex terrain using statistical models (vol 7, 013103, 2015) SO JOURNAL OF RENEWABLE AND SUSTAINABLE ENERGY LA English DT Correction C1 [Bulaevskaya, V.; Wharton, S.; Miller, W. O.] Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. [Clifton, A.] Natl Renewable Energy Lab, Golden, CO 80401 USA. [Qualley, G.] Infigen Energy, Dallas, TX 75206 USA. RP Bulaevskaya, V (reprint author), Lawrence Livermore Natl Lab, POB 808,L-211, Livermore, CA 94551 USA. EM verab@llnl.gov NR 1 TC 0 Z9 0 U1 0 U2 2 PU AMER INST PHYSICS PI MELVILLE PA 1305 WALT WHITMAN RD, STE 300, MELVILLE, NY 11747-4501 USA SN 1941-7012 J9 J RENEW SUSTAIN ENER JI J. Renew. Sustain. Energy PD JAN PY 2015 VL 7 IS 1 AR 019901 DI 10.1063/1.4906780 PG 1 WC GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY; Energy & Fuels SC Science & Technology - Other Topics; Energy & Fuels GA CC7LJ UT WOS:000350548700042 ER PT J AU Bulaevskaya, V Wharton, S Clifton, A Qualley, G Miller, WO AF Bulaevskaya, V. Wharton, S. Clifton, A. Qualley, G. Miller, W. O. TI Wind power curve modeling in complex terrain using statistical models SO JOURNAL OF RENEWABLE AND SUSTAINABLE ENERGY LA English DT Article ID TURBINE POWER; ATMOSPHERIC STABILITY; SPEED AB The simplest power curves model wind power only as a function of the wind speed at the turbine hub height. While the latter is an essential predictor of power output, wind speed information in other parts of the vertical profile, as well as additional atmospheric variables, are also important determinants of power. The goal of this work was to determine the gain in predictive ability afforded by adding wind speed information at other heights, as well as other atmospheric variables, to the power prediction model. Using data from a wind farm with a moderately complex terrain in the Altamont Pass region in California, we trained three statistical models-a neural network, a random forest and a Gaussian process model-to predict power output from various sets of aforementioned predictors. The comparison of these predictions to the observed power data revealed that considerable improvements in prediction accuracy can be achieved both through the addition of predictors other than the hub-height wind speed and the use of statistical models. To our knowledge, the use of the Gaussian process model in this context is new, in contrast to neural networks and random forests. The advantage of this model over the other two models is that it provides a much more natural way to estimate the uncertainty associated with its predictions. In addition, this study presents one of the most comprehensive analyses to date of the relative importance of various wind power curve inputs. (C) 2015 AIP Publishing LLC. C1 [Bulaevskaya, V.; Wharton, S.; Miller, W. O.] Lawrence Livermore Natl Lab, Livermore, CA 94551 USA. [Clifton, A.] Natl Renewable Energy Lab, Golden, CO 80401 USA. [Qualley, G.] Infigen Energy, Dallas, TX 75206 USA. RP Bulaevskaya, V (reprint author), Lawrence Livermore Natl Lab, POB 808,L-211, Livermore, CA 94551 USA. EM verab@llnl.gov FU U.S. Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07NA27344]; LLNL Laboratory Directed Research and Development (LDRD) [12-ER-069] FX This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under the Contract No. DE-AC52-07NA27344 and funded by the LLNL Laboratory Directed Research and Development (LDRD) Grant No. 12-ER-069. The authors are extremely grateful for Infigen Energy's partnership, including data sharing, intellectual input and field campaign assistance. The authors would also like to thank Cary Gellner, Maureen Alai, and John Van Fossen (LLNL) for building the solar panel/battery arrays, Jennifer Newman (Univ. of Oklahoma) for assistance in the lidar deployments, and Matthew Simpson, Donald Lucas, Gardar Johannesson (LLNL) and the anonymous reviewers for valuable comments on an earlier version of this manuscript. NR 61 TC 7 Z9 7 U1 1 U2 11 PU AMER INST PHYSICS PI MELVILLE PA 1305 WALT WHITMAN RD, STE 300, MELVILLE, NY 11747-4501 USA SN 1941-7012 J9 J RENEW SUSTAIN ENER JI J. Renew. Sustain. Energy PD JAN PY 2015 VL 7 IS 1 AR 013103 DI 10.1063/1.4904430 PG 24 WC GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY; Energy & Fuels SC Science & Technology - Other Topics; Energy & Fuels GA CC7LJ UT WOS:000350548700009 ER PT J AU Gonzalez, DL Angus, MP Tetteh, IK Bello, GA Padmanabhan, K Pendse, SV Srinivas, S Yu, J Semazzi, F Kumar, V Samatova, NF AF Gonzalez, D. L., II Angus, M. P. Tetteh, I. K. Bello, G. A. Padmanabhan, K. Pendse, S. V. Srinivas, S. Yu, J. Semazzi, F. Kumar, V. Samatova, N. F. TI On the data-driven inference of modulatory networks in climate science: an application to West African rainfall SO NONLINEAR PROCESSES IN GEOPHYSICS LA English DT Article ID TROPICAL ATLANTIC; INDIAN-OCEAN; VARIABILITY; SAHEL; DYNAMICS; ASSOCIATION; IMPACTS; SYSTEMS; REGION; LASSO AB Decades of hypothesis-driven and/or first-principles research have been applied towards the discovery and explanation of the mechanisms that drive climate phenomena, such as western African Sahel summer rainfall variability. Although connections between various climate factors have been theorized, not all of the key relationships are fully understood. We propose a data-driven approach to identify candidate players in this climate system, which can help explain underlying mechanisms and/or even suggest new relationships, to facilitate building a more comprehensive and predictive model of the modulatory relationships influencing a climate phenomenon of interest. We applied coupled heterogeneous association rule mining (CHARM), Lasso multivariate regression, and dynamic Bayesian networks to find relationships within a complex system, and explored means with which to obtain a consensus result from the application of such varied methodologies. Using this fusion of approaches, we identified relationships among climate factors that modulate Sahel rainfall. These relationships fall into two categories: well-known associations from prior climate knowledge, such as the relationship with the El Nino-Southern Oscillation (ENSO) and putative links, such as North Atlantic Oscillation, that invite further research. C1 [Gonzalez, D. L., II; Angus, M. P.; Tetteh, I. K.; Bello, G. A.; Padmanabhan, K.; Pendse, S. V.; Srinivas, S.; Yu, J.; Semazzi, F.; Samatova, N. F.] N Carolina State Univ, Raleigh, NC 27695 USA. [Gonzalez, D. L., II; Bello, G. A.; Padmanabhan, K.; Pendse, S. V.; Srinivas, S.; Samatova, N. F.] Oak Ridge Natl Lab, Oak Ridge, TN 37831 USA. [Kumar, V.] Univ Minnesota, Minneapolis, MN 55455 USA. RP Samatova, NF (reprint author), N Carolina State Univ, Raleigh, NC 27695 USA. EM samatova@csc.ncsu.edu FU US Department of Energy, Office of Science, the Office of Advanced Scientific Computing Research (SDAVI Institute); US National Science Foundation (Expeditions in Computing program); US D.O.E. [DEAC05-00OR22725] FX This work was supported in part by the US Department of Energy, Office of Science, the Office of Advanced Scientific Computing Research (SDAVI Institute), and the US National Science Foundation (Expeditions in Computing program). Oak Ridge National Laboratory is managed by UT-Battelle for the LLC US D.O.E. under contract no. DEAC05-00OR22725. Any opinions, findings, and conclusions or recommendations expressed in this material are those of the authors and do not necessarily reflect the views of the National Science Foundation. NR 48 TC 0 Z9 0 U1 3 U2 9 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1023-5809 J9 NONLINEAR PROC GEOPH JI Nonlinear Process Geophys. PY 2015 VL 22 IS 1 BP 33 EP 46 DI 10.5194/npg-22-33-2015 PG 14 WC Geochemistry & Geophysics; Meteorology & Atmospheric Sciences SC Geochemistry & Geophysics; Meteorology & Atmospheric Sciences GA CC7NU UT WOS:000350555800003 ER PT J AU Kuzkin, V Krivtsov, A Jones, R Zimmerman, J AF Kuzkin, V. A. Krivtsov, A. M. Jones, R. E. Zimmerman, J. A. TI Material frame representation of equivalent stress tensor for discrete solids SO PHYSICAL MESOMECHANICS LA English DT Article DE Cauchy stress tensor; material frame formulation; molecular dynamics ID MOLECULAR-DYNAMICS; SIMULATIONS; CRYSTALS; STATE AB In this paper, we derive expressions for equivalent Cauchy and Piola stress tensors that can be applied to discrete solids and are exact for the case of homogeneous deformation. The main principles used for this derivation are material frame formulation, long wave approximation and decomposition of particle motion into continuum and thermal parts. Equivalent Cauchy and Piola stress tensors for discrete solids are expressed in terms of averaged interparticle distances and forces. No assumptions about interparticle forces are used in the derivation, thereby ensuring our expressions are valid irrespective of the choice of interatomic potential used to model the discrete solid. The derived expressions are used for calculation of the local Cauchy stress in several test problems. The results are compared with prediction of the classical continuum definition (force per unit area) as well as existing discrete formulations (Hardy, Lucy, and Heinz-Paul-Binder stress tensors). It is shown that in the case of homogeneous deformations and finite temperatures the proposed expression leads to the same values of stresses as classical continuum definition. Hardy and Lucy stress tensors give the same result only if the stress is averaged over a sufficiently large volume. Thus, given the lack of sensitivity to averaging volume size, the derived expressions can be used as benchmarks for calculation of stresses in discrete solids. C1 [Kuzkin, V. A.; Krivtsov, A. M.] Russian Acad Sci, Inst Problems Mech Engn, St Petersburg 199178, Russia. [Kuzkin, V. A.; Krivtsov, A. M.] St Petersburg State Polytech Univ, St Petersburg 195251, Russia. [Jones, R. E.; Zimmerman, J. A.] Sandia Natl Labs, Livermore, CA 94551 USA. RP Kuzkin, V (reprint author), Russian Acad Sci, Inst Problems Mech Engn, St Petersburg 199178, Russia. EM kuzkinva@gmail.com RI Krivtsov, Anton-Irzhi/P-3013-2016; Kuzkin, Vitaliy /E-9407-2017 OI Kuzkin, Vitaliy /0000-0003-0484-0106 FU Sandia National Laboratories; RSCF [14-11-00599] FX The authors are deeply grateful to Prof. William Graham Hoover for the fruitful discussions of the present paper. This work was financially supported by Sandia National Laboratories and RSCF (grant No. 14-11-00599). NR 37 TC 2 Z9 3 U1 2 U2 8 PU SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013 USA SN 1029-9599 EI 1990-5424 J9 PHYS MESOMECH JI Phys. Mesomech. PD JAN PY 2015 VL 18 IS 1 BP 13 EP 23 DI 10.1134/S1029959915010038 PG 11 WC Mechanics; Materials Science, Characterization & Testing SC Mechanics; Materials Science GA CC6PK UT WOS:000350487800003 ER PT J AU Carino, EV Diesendruck, CE Moore, JS Curtiss, LA Assary, RS Brushett, FR AF Carino, Emily V. Diesendruck, Charles E. Moore, Jeffrey S. Curtiss, Larry A. Assary, Rajeev S. Brushett, Fikile R. TI BF3-promoted electrochemical properties of quinoxaline in propylene carbonate SO RSC ADVANCES LA English DT Article ID DENSITY-FUNCTIONAL THEORY; REDOX FLOW BATTERY; RESEARCH-AND-DEVELOPMENT; SOLVATION FREE-ENERGIES; LI-ION CELLS; DI-N-OXIDES; OXIDATION POTENTIALS; LIPF6-BASED ELECTROLYTES; DECOMPOSITION REACTIONS; REDUCTION POTENTIALS AB Electrochemical and density functional studies demonstrate that coordination of electrolyte constituents to quinoxalines modulates their electrochemical properties. Quinoxalines are shown to be electrochemically inactive in most electrolytes in propylene carbonate, yet the predicted reduction potential is shown to match computational estimates in acetonitrile. We find that in the presence of LiBF4 and trace water, an adduct is formed between quinoxaline and the Lewis acid BF3, which then displays electrochemical activity at 1-1.5 V higher than prior observations of quinoxaline electrochemistry in non-aqueous media. Direct synthesis and testing of a bis-BF3 quinoxaline complex further validates the assignment of the electrochemically active species, presenting up to a similar to 26-fold improvement in charging capacity, demonstrating the advantages of this adduct over unmodified quinoxaline in LiBF4-based electrolyte. The use of Lewis acids to effectively "turn on" the electrochemical activity of organic molecules may lead to the development of new active material classes for energy storage applications. C1 [Carino, Emily V.; Diesendruck, Charles E.; Moore, Jeffrey S.; Curtiss, Larry A.; Assary, Rajeev S.; Brushett, Fikile R.] Joint Ctr Energy Storage Res, Argonne, IL 60439 USA. [Carino, Emily V.; Brushett, Fikile R.] MIT, Dept Chem Engn, Cambridge, MA 02139 USA. [Diesendruck, Charles E.; Moore, Jeffrey S.] Univ Illinois, Dept Chem, Urbana, IL 61801 USA. [Curtiss, Larry A.; Assary, Rajeev S.] Argonne Natl Lab, Div Mat Sci, Argonne, IL 60439 USA. RP Assary, RS (reprint author), Joint Ctr Energy Storage Res, Argonne, IL 60439 USA. EM assary@anl.gov; brushett@mit.edu RI Surendran Assary, Rajeev/E-6833-2012; OI Surendran Assary, Rajeev/0000-0002-9571-3307; Diesendruck, Charles/0000-0001-5576-1366 FU Joint Center for Energy Storage Research, an Energy Innovation Hub - U.S. Department of Energy, Office of Science, Basic Energy Sciences; U. S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357] FX This work was supported as part of the Joint Center for Energy Storage Research, an Energy Innovation Hub funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences. We gratefully acknowledge the computing resources provided on "Blues," a 320-node computing cluster operated by the Laboratory Computing Resource Center at Argonne National Laboratory. 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. NR 44 TC 9 Z9 9 U1 2 U2 17 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2046-2069 J9 RSC ADV JI RSC Adv. PY 2015 VL 5 IS 24 BP 18822 EP 18831 DI 10.1039/c5ra00137d PG 10 WC Chemistry, Multidisciplinary SC Chemistry GA CC0BE UT WOS:000349999200079 ER PT J AU Yi, D Yang, L Xie, SJ Saxena, A AF Yi, Ding Yang, Liu Xie, Shijie Saxena, Avadh TI Stability of hydrogenated graphene: a first-principles study SO RSC ADVANCES LA English DT Article ID REVERSIBLE HYDROGENATION; BILAYER GRAPHENE; NANORIBBONS; GRAPHONE; GRAPHANE AB In order to explain the disagreement between present theoretical and experimental investigations on the stability of hydrogenated graphene, we have systematically studied hydrogenated graphene with different configurations from the consideration of single-side and double-side adsorption using first-principles calculations. Both binding energy and formation energy are calculated to characterize the stability of the system. It is found that single-side hydrogenated graphene is always unstable. However, for double-side hydrogenation, some configurations are stable due to the increased carbon-carbon sp(3) hybridization compared to single-side hydrogenation. Furthermore, it is found that the system is energetically favorable when an equal number of hydrogen atoms are adsorbed on each side of the graphene. C1 [Yi, Ding; Yang, Liu; Xie, Shijie] Shandong Univ, Sch Phys, State Key Lab Crystal Mat, Jinan 250100, Peoples R China. [Saxena, Avadh] Los Alamos Natl Lab, Div Theoret, Los Alamos, NM 87545 USA. RP Xie, SJ (reprint author), Shandong Univ, Sch Phys, State Key Lab Crystal Mat, Jinan 250100, Peoples R China. EM xsj@sdu.edu.cn FU National Natural Science Foundation of the People's Republic of China [11174181, 21161160445]; 111 project [B13029]; U.S. Department of Energy FX The authors thank Prof. Nujiang Tang of Nanjing University and Dr Qian Feng of Fujian Normal University for the useful discussions and suggestions. This work was financially supported by the National Natural Science Foundation of the People's Republic of China (Grant no. 11174181 and no. 21161160445) and 111 project B13029. This work was also supported in part by the U.S. Department of Energy. NR 32 TC 6 Z9 7 U1 11 U2 37 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2046-2069 J9 RSC ADV JI RSC Adv. PY 2015 VL 5 IS 26 BP 20617 EP 20622 DI 10.1039/c5ra00004a PG 6 WC Chemistry, Multidisciplinary SC Chemistry GA CC3BW UT WOS:000350220400100 ER PT J AU Kumar, R Lokitz, BS Sides, SW Chen, JH Heller, WT Ankner, JF Browning, JF Kilbey, SM Sumpter, BG AF Kumar, Rajeev Lokitz, Bradley S. Sides, Scott W. Chen, Jihua Heller, William T. Ankner, John F. Browning, James F. Kilbey, S. Michael, II Sumpter, Bobby G. TI Microphase separation in thin films of lamellar forming polydisperse di-block copolymers SO RSC ADVANCES LA English DT Article ID ABA TRIBLOCK COPOLYMERS; CARLO PHASE-DIAGRAM; DIBLOCK COPOLYMERS; CONFORMATIONAL ASYMMETRY; NEUTRON REFLECTIVITY; X-RAY; MELTS; MORPHOLOGY; POLYMERS; TRANSITION AB Despite the ubiquity of polydispersity in chain lengths of di-block copolymers, its effects on microphase separation in thin films have eluded a clear understanding. In this work, we have studied effects of polydispersity on the microphase separation in thin films of lamellar forming di-block copolymers using self-consistent field theory (SCFT) and neutron reflectivity experiments. Di-block copolymers containing a polydisperse block of poly(glycidylmethacrylate) (PGMA) connected to a near-monodisperse block poly(2-vinyl-4,4-dimethyl-d(6) azlactone) (PVDMA-d(6)) are considered in this work. Effects of chain length polydispersity, film thickness, substrate-monomer and monomer-monomer interactions on the microphase segregation are studied using SCFT. The theoretical study reveals that in comparison to a film created with monodisperse di-block copolymers, an increase in polydispersity tends to decrease the number of lamellar strata that can be packed in a film of given thickness. This is a direct consequence of an increase in lamellar domain spacing with an increase in polydispersity index. Furthermore, it is shown that polydispersity induces conformational asymmetry and an increase in the polydispersity index leads to an increase in the effective Kuhn segment length of the polydisperse blocks. It is shown that the conformational asymmetry effects, which are entropic in origin and of increasing importance as film thickness decreases, drive the polydisperse blocks to the middle of the films despite favorable substrate interactions. These predictions are verified by results from neutron reflectivity experiments on thin films made from moderately polydisperse PGMA-PVDMA-d(6) di-block copolymer deposited on silicon substrates. Finally, results from SCFT are used to predict neutron reflectivity profiles, providing a facile and robust route to obtain useful physical insights into the structure of polydisperse diblock copolymers at interfaces. C1 [Kumar, Rajeev; Sumpter, Bobby G.] Oak Ridge Natl Lab, Div Math & Comp Sci, Oak Ridge, TN 37831 USA. [Kumar, Rajeev; Lokitz, Bradley S.; Chen, Jihua; Sumpter, Bobby G.] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA. [Sides, Scott W.] Natl Renewable Energy Lab, Golden, CO 80401 USA. [Heller, William T.; Ankner, John F.; Browning, James F.] Oak Ridge Natl Lab, Spallat Neutron Source, Oak Ridge, TN 37831 USA. [Kilbey, S. Michael, II] Univ Tennessee, Dept Chem, Knoxville, TN 37996 USA. RP Kumar, R (reprint author), Oak Ridge Natl Lab, Div Math & Comp Sci, Oak Ridge, TN 37831 USA. EM kumarr@ornl.gov RI Chen, Jihua/F-1417-2011; Sumpter, Bobby/C-9459-2013; Kumar, Rajeev/Q-2255-2015; Lokitz, Bradley/Q-2430-2015; Browning, James/C-9841-2016 OI Chen, Jihua/0000-0001-6879-5936; Sumpter, Bobby/0000-0001-6341-0355; Ankner, John/0000-0002-6737-5718; Kumar, Rajeev/0000-0001-9494-3488; Lokitz, Bradley/0000-0002-1229-6078; Browning, James/0000-0001-8379-259X FU Oak Ridge National Laboratory (ORNL) by the Scientific User Facilities Division, Office of Basic Energy Sciences; U.S. Department of Energy; National Science Foundation [1133320]; Laboratory Directed Research and Development (LDRD) at ORNL; Scientific User Facilities Division, Office of Basic Energy Sciences, US Department of Energy; Office of Science of the U.S. Department of Energy [DE-AC05-00OR22725] FX This research was conducted in part at the Center for Nanophase Materials Sciences (CNMS), which is sponsored at Oak Ridge National Laboratory (ORNL) by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. SMKII acknowledges support from the National Science Foundation (Award no. 1133320). This work was supported by Laboratory Directed Research and Development (LDRD) at ORNL. Research conducted at ORNL's Spallation Neutron Source was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, US Department of Energy. The computations were performed using the resources of the CNMS and Oak Ridge Leadership Computing Facility at ORNL, which is supported by the Office of Science of the U.S. Department of Energy under Contract no. DE-AC05-00OR22725. NR 49 TC 5 Z9 5 U1 10 U2 42 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2046-2069 J9 RSC ADV JI RSC Adv. PY 2015 VL 5 IS 27 BP 21336 EP 21348 DI 10.1039/c5ra00974j PG 13 WC Chemistry, Multidisciplinary SC Chemistry GA CC3CH UT WOS:000350221600090 ER PT J AU Cahill, JF Fei, H Cohen, SM Prather, KA AF Cahill, J. F. Fei, H. Cohen, S. M. Prather, K. A. TI Characterization of core-shell MOF particles by depth profiling experiments using on-line single particle mass spectrometry SO ANALYST LA English DT Article ID METAL-ORGANIC FRAMEWORKS; COORDINATION POLYMER CRYSTALS; POSTSYNTHETIC LIGAND; FUNCTIONALIZATION; NANOPARTICLES; NANOSCALE; DESORPTION/IONIZATION; FABRICATION; MORPHOLOGY; AMMONIUM AB Materials with core-shell structures have distinct properties that lend themselves to a variety of potential applications. Characterization of small particle core-shell materials presents a unique analytical challenge. Herein, single particles of solid-state materials with core-shell structures were measured using on-line aerosol time-of-flight mass spectrometry (ATOFMS). Laser 'depth profiling' experiments verified the core-shell nature of two known core-shell particle configurations (< 2 mu m diameter) that possessed inverted, complimentary core-shell compositions (ZrO2@SiO2 versus SiO2@ZrO2). The average peak area ratios of Si and Zr ions were calculated to definitively show their core-shell composition. These ratio curves acted as a calibrant for an uncharacterized sample - a metal-organic framework (MOF) material surround by silica (UiO-66(Zr)@SiO2; UiO = University of Oslo). ATOFMS depth profiling was used to show that these particles did indeed exhibit a core-shell architecture. The results presented here show that ATOFMS can provide unique insights into core-shell solid-state materials with particle diameters between 0.2-3 mu m. C1 [Cahill, J. F.] Oak Ridge Natl Lab, Div Chem Sci, Organ & Biol Mass Spectrometry Grp, Oak Ridge, TN 37831 USA. [Fei, H.; Cohen, S. M.; Prather, K. A.] Univ Calif San Diego, Dept Chem & Biochem, La Jolla, CA 92093 USA. [Prather, K. A.] Univ Calif San Diego, Scripps Inst Oceanog, La Jolla, CA 92093 USA. RP Prather, KA (reprint author), Univ Calif San Diego, Dept Chem & Biochem, La Jolla, CA 92093 USA. EM kprather@ucsd.edu RI Fei, Honghan/D-6124-2015; Fei, Honghan/G-3445-2011 OI Cahill, John/0000-0002-9866-4010; Fei, Honghan/0000-0003-1353-9921 FU National Science Foundation, Division of Materials Research [DMR-1262226] FX The funding for this work was provided by a grant from the National Science Foundation, Division of Materials Research (DMR-1262226). NR 37 TC 1 Z9 1 U1 12 U2 118 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 0003-2654 EI 1364-5528 J9 ANALYST JI Analyst PY 2015 VL 140 IS 5 BP 1510 EP 1515 DI 10.1039/c4an01913j PG 6 WC Chemistry, Analytical SC Chemistry GA CB7VS UT WOS:000349837200018 PM 25587577 ER PT J AU Wang, M Xu, B Cao, J Tie, X Wang, H Zhang, R Qian, Y Rasch, PJ Zhao, S Wu, G Zhao, H Joswiak, DR Li, J Xie, Y AF Wang, M. Xu, B. Cao, J. Tie, X. Wang, H. Zhang, R. Qian, Y. Rasch, P. J. Zhao, S. Wu, G. Zhao, H. Joswiak, D. R. Li, J. Xie, Y. TI Carbonaceous aerosols recorded in a southeastern Tibetan glacier: analysis of temporal variations and model estimates of sources and radiative forcing SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID LIGHT-ABSORBING IMPURITIES; ATMOSPHERIC BROWN CLOUDS; BLACK-CARBON; ORGANIC-CARBON; ARCTIC SNOW; HYDROLOGICAL CYCLE; OPTICAL-PROPERTIES; SPECTRAL ALBEDO; SULFUR-DIOXIDE; RURAL INDIA AB High temporal resolution measurements of black carbon (BC) and organic carbon (OC) covering the time period of 1956-2006 in an ice core over the southeastern Tibetan Plateau show a distinct seasonal dependence of BC and OC with higher respective concentrations but a lower OC / BC ratio in the non-monsoon season than during the summer monsoon. We use a global aerosol-climate model, in which BC emitted from different source regions can be explicitly tracked, to quantify BC source-receptor relationships between four Asian source regions and the southeastern Tibetan Plateau as a receptor. The model results show that South Asia has the largest contribution to the presentday (1996-2005) mean BC deposition at the ice-core drilling site during the non-monsoon season (October to May) (81 %) and all year round (74 %), followed by East Asia (14% to the non-monsoon mean and 21% to the annual mean). The ice-core record also indicates stable and relatively low BC and OC deposition fluxes from the late 1950s to 1980, followed by an overall increase to recent years. This trend is consistent with the BC and OC emission inventories and the fuel consumption of South Asia (as the primary contributor to annual mean BC deposition). Moreover, the increasing trend of the OC / BC ratio since the early 1990s indicates a growing contribution of coal combustion and/or biomass burning to the emissions. The estimated radiative forcing induced by BC and OC impurities in snow has increased since 1980, suggesting an increasing potential influence of carbonaceous aerosols on the Tibetan glacier melting and the availability of water resources in the surrounding regions. Our study indicates that more attention to OC is merited because of its non-negligible light absorption and the recent rapid increases evident in the ice-core record. C1 [Wang, M.; Xu, B.; Wu, G.; Zhao, H.; Joswiak, D. R.; Li, J.; Xie, Y.] Chinese Acad Sci, Inst Tibetan Plateau Res, Key Lab Tibetan Environm Changes & Land Surface P, Beijing 100101, Peoples R China. [Wang, M.; Wang, H.; Zhang, R.; Qian, Y.; Rasch, P. J.] PNNL, Atmospher Sci & Global Change Div, Richland, WA 99352 USA. [Cao, J.; Tie, X.; Zhao, S.] Chinese Acad Sci, Inst Earth Environm, State Key Lab Loess & Quaternary Geol, Beijing 100085, Peoples R China. [Tie, X.] Natl Ctr Atmospher Res, Boulder, CO 80303 USA. [Zhang, R.] Lanzhou Univ, Coll Atmospher Sci, Key Lab Semiarid Climate Change, Minist Educ, Lanzhou 730000, Gansu, Peoples R China. RP Wang, M (reprint author), Chinese Acad Sci, Inst Tibetan Plateau Res, Key Lab Tibetan Environm Changes & Land Surface P, Beijing 100101, Peoples R China. EM wangmo@itpcas.ac.cn RI qian, yun/E-1845-2011; Wang, Hailong/B-8061-2010; Cao, Junji/D-3259-2014 OI Wang, Hailong/0000-0002-1994-4402; Cao, Junji/0000-0003-1000-7241 FU China National Funds for Distinguished Young Scientists; National Natural Science Foundation of China [41125003, 41101063, 2009CB723901]; US Department of Energy (DOE), Office of Science, Biological and Environmental Research as part of the Earth System Modeling program; China Scholarship Fund; DOE by Battelle Memorial Institute [DE-AC05-76RLO1830]; National Science Foundation FX This work was supported by the China National Funds for Distinguished Young Scientists and the National Natural Science Foundation of China, including 41125003, 41101063, and 2009CB723901. H. Wang, Y. Qian and P. J. Rasch were supported by the US Department of Energy (DOE), Office of Science, Biological and Environmental Research as part of the Earth System Modeling program. R. Zhang acknowledges support from the China Scholarship Fund. PNNL is operated for DOE by Battelle Memorial Institute under contract DE-AC05-76RLO1830. The National Center for Atmospheric Research is sponsored by the National Science Foundation. We thank Z. Guo and S. Yang for providing the observations of snow. NR 85 TC 13 Z9 17 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 2015 VL 15 IS 3 BP 1191 EP 1204 DI 10.5194/acp-15-1191-2015 PG 14 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA CB7IF UT WOS:000349799500004 ER PT J AU Lowe, D Archer-Nicholls, S Morgan, W Allan, J Utembe, S Ouyang, B Aruffo, E Le Breton, M Zaveri, RA Di Carlo, P Percival, C Coe, H Jones, R McFiggans, G AF Lowe, D. Archer-Nicholls, S. Morgan, W. Allan, J. Utembe, S. Ouyang, B. Aruffo, E. Le Breton, M. Zaveri, R. A. Di Carlo, P. Percival, C. Coe, H. Jones, R. McFiggans, G. TI WRF-Chem model predictions of the regional impacts of N2O5 heterogeneous processes on night-time chemistry over north-western Europe SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID INTERMEDIATES CRI MECHANISM; SECONDARY ORGANIC AEROSOL; SIZE DISTRIBUTIONS; ATMOSPHERIC CHEMISTRY; MASS-SPECTROMETER; O-X; NITRATE; PARAMETERIZATION; NO3; REANALYSIS AB Chemical modelling studies have been conducted over north-western Europe in summer conditions, showing that night-time dinitrogen pentoxide (N2O5) heterogeneous reactive uptake is important regionally in modulating particulate nitrate and has a modest influence on oxidative chemistry. Results from Weather Research and Forecasting model with Chemistry (WRF-Chem) model simulations, run with a detailed volatile organic compound (VOC) gas-phase chemistry scheme and the Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) sectional aerosol scheme, were compared with a series of airborne gas and particulate measurements made over the UK in July 2010. Modelled mixing ratios of key gas-phase species were reasonably accurate (correlations with measurements of 0.7-0.9 for NO2 and O-3). However modelled loadings of particulate species were less accurate (correlation with measurements for particulate sulfate and ammonium were between 0.0 and 0.6). Sulfate mass loadings were particularly low (modelled means of 0.5-0.7 mu gkg(air)(-1), compared with measurements of 1.0-1.5 mu gkg(air)(-1)). Two flights from the campaign were used as test cases - one with low relative humidity (RH) (60-70 %), the other with high RH (80-90 %). N2O5 heterogeneous chemistry was found to not be important in the low-RH test case; but in the high-RH test case it had a strong effect and significantly improved the agreement between modelled and measured NO3 and N2O5. When the model failed to capture atmospheric RH correctly, the modelled NO3 and N2O5 mixing ratios for these flights differed significantly from the measurements. This demonstrates that, for regional modelling which involves heterogeneous processes, it is essential to capture the ambient temperature and water vapour profiles. The night-time NO3 oxidation of VOCs across the whole region was found to be 100-300 times slower than the day-time OH oxidation of these compounds. The difference in contribution was less for alkenes (x80) and comparable for dimethylsulfide (DMS). However the suppression of NO3 mixing ratios across the domain by N2O5 heterogeneous chemistry has only a very slight, negative, influence on this oxidative capacity. The influence on regional particulate nitrate mass loadings is stronger. Night-time N2O5 heterogeneous chemistry maintains the production of particulate nitrate within polluted regions: when this process is taken into consideration, the daytime peak (for the 95th percentile) of PM10 nitrate mass loadings remains around 5.6 mu gkg(air)(-1), but the night-time minimum increases from 3.5 to 4.6 mu gkg(air)(-1). The sustaining of higher particulate mass loadings through the night by this process improves model skill at matching measured aerosol nitrate diurnal cycles and will negatively impact on regional air quality, requiring this process to be included in regional models. C1 [Lowe, D.; Archer-Nicholls, S.; Morgan, W.; Allan, J.; Le Breton, M.; Percival, C.; Coe, H.; McFiggans, G.] Univ Manchester, Sch Earth Atmospher & Environm Sci, Manchester, Lancs, England. [Allan, J.] Univ Manchester, Natl Ctr Atmospher Sci, Manchester, Lancs, England. [Utembe, S.] Univ Melbourne, Sch Earth Sci, Melbourne, Vic 3010, Australia. [Ouyang, B.; Jones, R.] Univ Cambridge, Dept Chem, Cambridge CB2 1EW, England. [Aruffo, E.; Di Carlo, P.] Univ Aquila, Dipartimento Fis, CETEMPS, I-67100 Laquila, Italy. [Zaveri, R. A.] Pacific NW Natl Lab, Atmospher Sci & Global Change Div, Richland, WA 99352 USA. RP McFiggans, G (reprint author), Univ Manchester, Sch Earth Atmospher & Environm Sci, Manchester, Lancs, England. EM g.mcfiggans@manchester.ac.uk RI McFiggans, Gordon/B-8689-2011; Di Carlo, Piero/C-1657-2016; Utembe, Steven/C-4713-2016; Zaveri, Rahul/G-4076-2014; Morgan, William/D-1690-2011; Di Carlo, Piero/Q-4450-2016; Allan, James/B-1160-2010; OI McFiggans, Gordon/0000-0002-3423-7896; Di Carlo, Piero/0000-0003-4971-4509; Utembe, Steven/0000-0002-2741-3142; Zaveri, Rahul/0000-0001-9874-8807; Di Carlo, Piero/0000-0003-4971-4509; Allan, James/0000-0001-6492-4876; percival, carl/0000-0003-2525-160X; Coe, Hugh/0000-0002-3264-1713 FU NERC RONOCO project [NE/F004656/1]; NERC quota studentship FX We would like to acknowledge the efforts of the whole RONOCO team during and after the project. Airborne data were obtained using the BAe 146-301 Atmospheric Research Aircraft (ARA) flown by Directflight Ltd and managed by the Facility for Airborne Atmospheric Measurements (FAAM), which is a joint entity of the Natural Environment Research Council (NERC) and the Met Office. The NERC National Centre for Atmospheric Science (NCAS) Atmospheric Measurement Facility (AMF) supported the maintenance of the cToF-AMS. NCAS also supported the development of the data interpretation methods employed here through its Composition Directorate. This work was supported by the NERC RONOCO project NE/F004656/1. S. Archer-Nicholls was supported by a NERC quota studentship. Model runs were carried out on the High-End Computing Terascale Resources (HECToR) British national supercomputer. NR 71 TC 3 Z9 3 U1 4 U2 39 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1680-7316 EI 1680-7324 J9 ATMOS CHEM PHYS JI Atmos. Chem. Phys. PY 2015 VL 15 IS 3 BP 1385 EP 1409 DI 10.5194/acp-15-1385-2015 PG 25 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA CB7IF UT WOS:000349799500016 ER PT J AU Shi, X Liu, X Zhang, K AF Shi, X. Liu, X. Zhang, K. TI Effects of pre-existing ice crystals on cirrus clouds and comparison between different ice nucleation parameterizations with the Community Atmosphere Model (CAM5) SO ATMOSPHERIC CHEMISTRY AND PHYSICS LA English DT Article ID TROPICAL TROPOPAUSE LAYER; MICROWAVE IMAGER SSM/I; LIQUID WATER; MICROPHYSICS SCHEME; AQUEOUS-SOLUTIONS; VERSION-3 CAM3; CLIMATE MODEL; AEROSOLS; NUCLEI; SENSITIVITY AB In order to improve the treatment of ice nucleation in a more realistic manner in the Community Atmosphere Model version 5.3 (CAM5.3), the effects of pre-existing ice crystals on ice nucleation in cirrus clouds are considered. In addition, by considering the in-cloud variability in ice saturation ratio, homogeneous nucleation takes place spatially only in a portion of the cirrus cloud rather than in the whole area of the cirrus cloud. Compared to observations, the ice number concentrations and the probability distributions of ice number concentration are both improved with the updated treatment. The pre-existing ice crystals significantly reduce ice number concentrations in cirrus clouds, especially at mid- to high latitudes in the upper troposphere (by a factor of similar to 10). Furthermore, the contribution of heterogeneous ice nucleation to cirrus ice crystal number increases considerably. Besides the default ice nucleation parameterization of Liu and Penner (2005, hereafter LP) in CAM5.3, two other ice nucleation parameterizations of Barahona and Nenes (2009, hereafter BN) and Karcher et al. (2006, hereafter KL) are implemented in CAM5.3 for the comparison. In-cloud ice crystal number concentration, percentage contribution from heterogeneous ice nucleation to total ice crystal number, and pre-existing ice effects simulated by the three ice nucleation parameterizations have similar patterns in the simulations with present-day aerosol emissions. However, the change (present-day minus pre-industrial times) in global annual mean column ice number concentration from the KL parameterization (3.24 x 10(6) m(-2)) is less than that from the LP (8.46 x 10(6) m(-2)) and BN (5.62 x 10(6) m(-2)) parameterizations. As a result, the experiment using the KL parameterization predicts a much smaller anthropogenic aerosol long-wave indirect forcing (0.24 W m(-2)) than that using the LP (0.46 W m(-2)) and BN (0.39W m(-2)) parameterizations. C1 [Shi, X.; Liu, X.] Univ Wyoming, Dept Atmospher Sci, Laramie, WY 82071 USA. [Shi, X.] Hebei Key Lab Meteorol & Ecoenvironm, Shijiazhuang, Peoples R China. [Shi, X.] Hebei Climate Ctr, Shijiazhuang, Peoples R China. [Zhang, K.] Pacific NW Natl Lab, Atmospher Sci & Global Change Div, Richland, WA 99352 USA. RP Liu, X (reprint author), Univ Wyoming, Dept Atmospher Sci, Laramie, WY 82071 USA. EM xliu6@uwyo.edu RI Liu, Xiaohong/E-9304-2011; Zhang, Kai/F-8415-2010 OI Liu, Xiaohong/0000-0002-3994-5955; Zhang, Kai/0000-0003-0457-6368 FU Office of Science of US Department of Energy as part of the Earth System Modeling Program; National Natural Science Foundation of China [41205071]; NCAR's Computational and Information Systems Laboratory; DOE by Battelle Memorial Institute [DE-AC05-76RL01830] FX X. Liu and K. Zhang were supported by the Office of Science of US Department of Energy as part of the Earth System Modeling Program. X. Shi would like to acknowledge the support from the National Natural Science Foundation of China (grant no. 41205071). We would like to acknowledge the use of computational resources (ark:/85065/d7wd3xhc) at the NCAR-Wyoming Supercomputing Center provided by the National Science Foundation and the State of Wyoming, and supported by NCAR's Computational and Information Systems Laboratory. PNNL is a multiprogram laboratory operated for DOE by Battelle Memorial Institute under contract DE-AC05-76RL01830. NR 85 TC 6 Z9 6 U1 1 U2 26 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1680-7316 EI 1680-7324 J9 ATMOS CHEM PHYS JI Atmos. Chem. Phys. PY 2015 VL 15 IS 3 BP 1503 EP 1520 DI 10.5194/acp-15-1503-2015 PG 18 WC Meteorology & Atmospheric Sciences SC Meteorology & Atmospheric Sciences GA CB7IF UT WOS:000349799500024 ER PT J AU Le Page, Y Morton, D Bond-Lamberty, B Pereira, JMC Hurtt, G AF Le Page, Y. Morton, D. Bond-Lamberty, B. Pereira, J. M. C. Hurtt, G. TI HESFIRE: a global fire model to explore the role of anthropogenic and weather drivers SO BIOGEOSCIENCES LA English DT Article ID BURNED AREA; FOREST-FIRES; VEGETATION MODEL; EARTH SYSTEM; EMISSIONS; CLIMATE; DEFORESTATION; SENSITIVITY; DYNAMICS; PATTERNS AB Vegetation fires are a major driver of ecosystem dynamics and greenhouse gas emissions. Anticipating potential changes in fire activity and their impacts relies first on a realistic model of fire activity (e.g., fire incidence and interannual variability) and second on a model accounting for fire impacts (e.g., mortality and emissions). In this paper, we focus on our understanding of fire activity and describe a new fire model, HESFIRE (Human-Earth System FIRE), which integrates the influence of weather, vegetation characteristics, and human activities on fires in a stand-alone framework. It was developed with a particular emphasis on allowing fires to spread over consecutive days given their major contribution to burned areas in many ecosystems. A subset of the model parameters was calibrated through an optimization procedure using observation data to enhance our knowledge of regional drivers of fire activity and improve the performance of the model on a global scale. Modeled fire activity showed reasonable agreement with observations of burned area, fire seasonality, and interannual variability in many regions, including for spatial and temporal domains not included in the optimization procedure. Significant discrepancies are investigated, most notably regarding fires in boreal regions and in xeric ecosystems and also fire size distribution. The sensitivity of fire activity to model parameters is analyzed to explore the dominance of specific drivers across regions and ecosystems. The characteristics of HESFIRE and the outcome of its evaluation provide insights into the influence of anthropogenic activities and weather, and their interactions, on fire activity. C1 [Le Page, Y.; Bond-Lamberty, B.] Univ Maryland, Pacific NW Natl Lab, Joint Global Change Res Inst, College Pk, MD 20740 USA. [Morton, D.] NASA, Goddard Space Flight Ctr, Greenbelt, MD 20771 USA. [Pereira, J. M. C.] Univ Lisbon, Inst Super Agron, Ctr Estudos Florestais, P-1349017 Lisbon, Portugal. [Hurtt, G.] Univ Maryland, Dept Geog Sci, College Pk, MD 20740 USA. RP Le Page, Y (reprint author), Univ Maryland, Pacific NW Natl Lab, Joint Global Change Res Inst, College Pk, MD 20740 USA. EM yannick.lepage@pnnl.gov RI Pereira, Jose/I-1283-2014; Bond-Lamberty, Ben/C-6058-2008; Morton, Douglas/D-5044-2012 OI Pereira, Jose/0000-0003-2583-3669; Bond-Lamberty, Ben/0000-0001-9525-4633; FU NASA Terrestrial Ecology and Inter-Disciplinary Studies programs; Office of Science of the U.S. Department of Energy; DOE [DE-AC05-76RL01830] FX The authors are grateful for research support provided by the NASA Terrestrial Ecology and Inter-Disciplinary Studies programs. The authors also wish to express appreciation to the Integrated Assessment Research Program in the Office of Science of the U.S. Department of Energy for partially funding this research. The Pacific Northwest National Laboratory is operated for DOE by Battelle Memorial Institute under contract DE-AC05-76RL01830. The views and opinions expressed in this paper are those of the authors alone. NR 60 TC 4 Z9 5 U1 3 U2 13 PU COPERNICUS GESELLSCHAFT MBH PI GOTTINGEN PA BAHNHOFSALLEE 1E, GOTTINGEN, 37081, GERMANY SN 1726-4170 EI 1726-4189 J9 BIOGEOSCIENCES JI Biogeosciences PY 2015 VL 12 IS 3 BP 887 EP 903 DI 10.5194/bg-12-887-2015 PG 17 WC Ecology; Geosciences, Multidisciplinary SC Environmental Sciences & Ecology; Geology GA CB7FU UT WOS:000349793100019 ER PT J AU Wei, H Yang, HB Ciesielski, PN Donohoe, BS McCann, MC Murphy, AS Peer, WA Ding, SY Himmel, ME Tucker, MP AF Wei, Hui Yang, Haibing Ciesielski, Peter N. Donohoe, Bryon S. McCann, Maureen C. Murphy, Angus S. Peer, Wendy A. Ding, Shi-You Himmel, Michael E. Tucker, Melvin P. TI Transgenic ferritin overproduction enhances thermochemical pretreatments in Arabidopsis SO BIOMASS & BIOENERGY LA English DT Article DE Ferritin; Iron accumulation; Transgenic Arabidopsis; Biomass saccharification; Dilute acid pretreatment; Prussian blue staining ID IRON HOMEOSTASIS ALTERATION; DILUTE-ACID PRETREATMENT; STEAM EXPLOSION; BINDING-PROTEIN; CORN STOVER; ACCUMULATION; BIOMASS; PLANTS; GENE; TEMPERATURE AB Reducing the severity of thermochemical pretreatment by incorporating iron ions as cocatalysts has been shown to enhance the sugar yield from dilute acid pretreatments and enzymatic saccharification. However, current approach of soaking iron containing acid solutions onto milled biomass prior to pretreatment is time-consuming and subject to diffusion limitations. Here, we overexpressed soybean ferritin protein intracellularly in Arabidopsis plants (referred to as FerIN) under the control of the 35S promoter for the purpose of accumulating iron ions in Arabidopsis plants. The transgenic Arabidopsis plants accumulated iron during growth under both normal and iron-augmented watering conditions. Prussian blue staining showed punctuate staining of iron predominantly on the interior surfaces of cell lumen in FerIN plants. The harvested transgenic biomass showed enhanced pretreatability, in that it released 13-19% more glucose and xylose than empty vector control plants. The data indicated a positive correlation between iron concentration and sugar release during pretreatment of transgenic biomass. (C) 2014 Elsevier Ltd. All rights reserved. C1 [Wei, Hui; Ciesielski, Peter N.; Donohoe, Bryon S.; Ding, Shi-You; Himmel, Michael E.] Natl Renewable Energy Lab, Biosci Ctr, Golden, CO 80401 USA. [Yang, Haibing; Murphy, Angus S.; Peer, Wendy A.] Purdue Univ, Dept Hort & Landscape Architecture, W Lafayette, IN 47907 USA. [McCann, Maureen C.] Purdue Univ, Dept Biol Sci, W Lafayette, IN 47907 USA. [Peer, Wendy A.] Univ Maryland, Dept Cellular & Mol Biosci, College Pk, MD 20742 USA. [Ding, Shi-You] Michigan State Univ, Dept Plant Biol, E Lansing, MI 48824 USA. [Tucker, Melvin P.] Natl Renewable Energy Lab, Natl Bioenergy Ctr, Golden, CO 80401 USA. RP Wei, H (reprint author), Natl Renewable Energy Lab, Biosci Ctr, 15013 Denver W Pkwy, Golden, CO 80401 USA. EM Hui.Wei@nrel.gov; Melvin.Tucker@nrel.gov RI Peer, Wendy/H-2970-2013 OI Peer, Wendy/0000-0003-0046-7324 FU Center for Direct Catalytic Conversion of Biomass to Biofuels (C3Bio); U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0000997]; U.S. Department of Energy [DE-AC36-08-GO28308] FX This work was supported by the Center for Direct Catalytic Conversion of Biomass to Biofuels (C3Bio), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Award Number DE-SC0000997. The National Renewable Energy Laboratory (NREL) is operated for the U.S. Department of Energy under Contract No. DE-AC36-08-GO28308. We thank Manjunatha Narayana Murthy, Troy Paddock and Xing-Ron Wu for the helpful discussions. Technical support from Zhenyu Wang and Fan Chen at The Samuel Roberts Noble Foundation is appreciated. NR 40 TC 5 Z9 5 U1 7 U2 16 PU PERGAMON-ELSEVIER SCIENCE LTD PI OXFORD PA THE BOULEVARD, LANGFORD LANE, KIDLINGTON, OXFORD OX5 1GB, ENGLAND SN 0961-9534 EI 1873-2909 J9 BIOMASS BIOENERG JI Biomass Bioenerg. PD JAN PY 2015 VL 72 BP 55 EP 64 DI 10.1016/j.biombioe.2014.11.022 PG 10 WC Agricultural Engineering; Biotechnology & Applied Microbiology; Energy & Fuels SC Agriculture; Biotechnology & Applied Microbiology; Energy & Fuels GA CB6FY UT WOS:000349724100007 ER PT J AU Jardine, K Yanez-Serrano, AM Williams, J Kunert, N Jardine, A Taylor, T Abrell, L Artaxo, P Guenther, A Hewitt, CN House, E Florentino, AP Manzi, A Higuchi, N Kesselmeier, J Behrendt, T Veres, PR Derstroff, B Fuentes, JD Martin, ST Andreae, MO AF Jardine, K. Yanez-Serrano, A. M. Williams, J. Kunert, N. Jardine, A. Taylor, T. Abrell, L. Artaxo, P. Guenther, A. Hewitt, C. N. House, E. Florentino, A. P. Manzi, A. Higuchi, N. Kesselmeier, J. Behrendt, T. Veres, P. R. Derstroff, B. Fuentes, J. D. Martin, S. T. Andreae, M. O. TI Dimethyl sulfide in the Amazon rain forest SO GLOBAL BIOGEOCHEMICAL CYCLES LA English DT Article DE dimethyl sulfide; DMS; Amazon ID VOLATILE SULFUR-COMPOUNDS; CARBONYL SULFIDE; TROPICAL FORESTS; MICROBIAL DECOMPOSITION; OCEANIC PHYTOPLANKTON; OXIDATION-PRODUCTS; ATMOSPHERIC SULFUR; EMISSIONS; AEROSOL; SOILS AB Surface-to-atmosphere emissions of dimethyl sulfide (DMS) may impact global climate through the formation of gaseous sulfuric acid, which can yield secondary sulfate aerosols and contribute to new particle formation. While oceans are generally considered the dominant sources of DMS, a shortage of ecosystem observations prevents an accurate analysis of terrestrial DMS sources. Using mass spectrometry, we quantified ambient DMS mixing ratios within and above a primary rainforest ecosystem in the central Amazon Basin in real-time (2010-2011) and at high vertical resolution (2013-2014). Elevated but highly variable DMS mixing ratios were observed within the canopy, showing clear evidence of a net ecosystem source to the atmosphere during both day and night in both the dry and wet seasons. Periods of high DMS mixing ratios lasting up to 8h (up to 160parts per trillion (ppt)) often occurred within the canopy and near the surface during many evenings and nights. Daytime gradients showed mixing ratios (up to 80ppt) peaking near the top of the canopy as well as near the ground following a rain event. The spatial and temporal distribution of DMS suggests that ambient levels and their potential climatic impacts are dominated by local soil and plant emissions. A soil source was confirmed by measurements of DMS emission fluxes from Amazon soils as a function of temperature and soil moisture. Furthermore, light- and temperature-dependent DMS emissions were measured from seven tropical tree species. Our study has important implications for understanding terrestrial DMS sources and their role in coupled land-atmosphere climate feedbacks. C1 [Jardine, K.] Lawrence Berkeley Natl Lab, Div Earth Sci, Climate Sci Dept, Berkeley, CA 94720 USA. [Yanez-Serrano, A. M.; Jardine, A.; Florentino, A. P.; Manzi, A.; Higuchi, N.] Natl Inst Amazon Res, Manaus, Amazonas, Brazil. [Williams, J.; Kesselmeier, J.; Behrendt, T.; Veres, P. R.; Derstroff, B.; Andreae, M. O.] Max Planck Inst Chem, Atmospher Chem Dept, D-55128 Mainz, Germany. [Williams, J.; Kesselmeier, J.; Behrendt, T.; Veres, P. R.; Derstroff, B.; Andreae, M. O.] Max Planck Inst Chem, Biogeochem Dept, D-55128 Mainz, Germany. [Kunert, N.] Max Planck Inst Biogeochem, D-07745 Jena, Germany. [Taylor, T.] Univ Arizona, Dept Ecol & Evolut Biol, Tucson, AZ 85721 USA. [Abrell, L.] Univ Arizona, Dept Chem, Tucson, AZ 85721 USA. [Abrell, L.] Univ Arizona, Dept Biochem, Tucson, AZ 85721 USA. [Abrell, L.] Univ Arizona, Dept Soil & Environm Sci, Tucson, AZ 85721 USA. [Abrell, L.] Univ Arizona, Dept Water & Environm Sci, Tucson, AZ 85721 USA. [Artaxo, P.] Univ Sao Paulo, Inst Phys, Sao Paulo, Brazil. [Guenther, A.] Pacific Northwest Natl Lab, Richland, WA USA. [Hewitt, C. N.; House, E.] Univ Lancaster, Lancaster Environm Ctr, Lancaster, England. [Fuentes, J. D.] Penn State Univ, Dept Meteorol, Coll Earth & Mineral Sci, University Pk, PA 16802 USA. [Martin, S. T.] Harvard Univ, Sch Engn & Appl Sci, Cambridge, MA 02138 USA. [Martin, S. T.] Harvard Univ, Dept Earth & Planetary Sci, Cambridge, MA 02138 USA. RP Jardine, K (reprint author), Lawrence Berkeley Natl Lab, Div Earth Sci, Climate Sci Dept, Berkeley, CA 94720 USA. EM kjjardine@lbl.gov RI Veres, Patrick/E-7441-2010; Martin, Scot/G-1094-2015; Kesselmeier, Jurgen/E-2389-2016; Artaxo, Paulo/E-8874-2010; Andreae, Meinrat/B-1068-2008; Jardine, Kolby/N-2802-2013 OI Abrell, Leif/0000-0003-2490-1180; Veres, Patrick/0000-0001-7539-353X; Martin, Scot/0000-0002-8996-7554; Kesselmeier, Jurgen/0000-0002-4446-534X; YANEZ SERRANO, ANA MARIA/0000-0001-6408-5961; Kunert, Norbert/0000-0002-5602-6221; Artaxo, Paulo/0000-0001-7754-3036; Andreae, Meinrat/0000-0003-1968-7925; Jardine, Kolby/0000-0001-8491-9310 FU Office of Science, Office of Biological and Environmental Research of the U.S. Department of Energy, Terrestrial Ecosystem Science Program [DE-AC02-05CH11231]; U.S. National Science Foundation through the AMAZON-PIRE (Partnerships for International Research and Education) award [0730305]; DFG [HALOPROC 763]; NERC CLAIRE-UK; German Max Planck Society; Fundacao de Amparo a Pesquisa do Estado de Sao Paulo FAPESP-AEROCLIMA 08/58100-2 [FAPESP-AEROCLIMA 08/58100-2] FX The data used in this manuscript are available for free download at www.archive.arm.gov. After logging in, registered users can find the data link under the "Get special data" submenu. This research was supported by the Director, Office of Science, Office of Biological and Environmental Research of the U.S. Department of Energy under contract DE-AC02-05CH11231 as part of their Terrestrial Ecosystem Science Program. Additional funding for this project came from the U.S. National Science Foundation through the AMAZON-PIRE (Partnerships for International Research and Education) award (0730305), DFG project HALOPROC 763, the NERC CLAIRE-UK project, and the German Max Planck Society. This work was also supported by Fundacao de Amparo a Pesquisa do Estado de Sao Paulo (FAPESP-AEROCLIMA 08/58100-2). We would like to thank several individuals at the Instituto Nacional de Pesquisas da Amazonia (INPA) in Manaus, Brazil, for logistics support including Veber Moura, Roberta Pereira de Souza, and Erika Schloemp. Finally, we kindly acknowledge Cor Becker for assistance in soil sampling from Suriname. NR 60 TC 10 Z9 10 U1 4 U2 31 PU AMER GEOPHYSICAL UNION PI WASHINGTON PA 2000 FLORIDA AVE NW, WASHINGTON, DC 20009 USA SN 0886-6236 EI 1944-9224 J9 GLOBAL BIOGEOCHEM CY JI Glob. Biogeochem. Cycle PD JAN PY 2015 VL 29 IS 1 BP 19 EP 32 DI 10.1002/2014GB004969 PG 14 WC Environmental Sciences; Geosciences, Multidisciplinary; Meteorology & Atmospheric Sciences SC Environmental Sciences & Ecology; Geology; Meteorology & Atmospheric Sciences GA CB8QB UT WOS:000349894600002 ER PT J AU Berdnikov, VV Somov, SV Pentchev, L Zihlmann, B AF Berdnikov, V. V. Somov, S. V. Pentchev, L. Zihlmann, B. TI A drift detector system with anode and cathode readout in the GlueX experiment SO INSTRUMENTS AND EXPERIMENTAL TECHNIQUES LA English DT Article AB A drift detector system designed to detect charged particle tracks in the GlueX experiment dedicated to study the nature of confinement is described. The key design features of the drift chambers associated with the requirement of a minimum material budget in the path of secondary particles are presented. The spatial resolution and the detection efficiency have been measured with cosmic rays using the automatic data acquisition system. C1 [Berdnikov, V. V.; Somov, S. V.] Natl Res Nucl Univ, Moscow Engn Phys Inst, Moscow 115409, Russia. [Pentchev, L.; Zihlmann, B.] Thomas Jefferson Natl Accelerator Facil, Newport News, VA 23606 USA. RP Berdnikov, VV (reprint author), Natl Res Nucl Univ, Moscow Engn Phys Inst, Kashirskoe Sh 31, Moscow 115409, Russia. EM vvberdnikov@gmail.com FU Jefferson Science Associated, LLC; U.S. DOE [DE-AC05-06OR23177] FX This work was performed by the National Research Nuclear University, Moscow Engineering Physics Institute, in collaboration with the Thomas Jefferson Accelerator Facility as a part of the GlueX experiment under financial support of the Jefferson Science Associated, LLC, which operates the Thomas Jefferson Accelerator Facility for the United States Department of Energy (U.S. DOE contract no. DE-AC05-06OR23177). NR 2 TC 4 Z9 4 U1 1 U2 3 PU MAIK NAUKA/INTERPERIODICA/SPRINGER PI NEW YORK PA 233 SPRING ST, NEW YORK, NY 10013-1578 USA SN 0020-4412 EI 1608-3180 J9 INSTRUM EXP TECH+ JI Instrum. Exp. Tech. PD JAN PY 2015 VL 58 IS 1 BP 25 EP 29 DI 10.1134/S0020441215010030 PG 5 WC Engineering, Multidisciplinary; Instruments & Instrumentation SC Engineering; Instruments & Instrumentation GA CB8NP UT WOS:000349887200004 ER PT S AU Server, WL Nanstad, RK AF Server, W. L. Nanstad, R. K. BE Soneda, N TI Reactor pressure vessel (RPV) design and fabrication: the case of the USA SO IRRADIATION EMBRITTLEMENT OF REACTOR PRESSURE VESSELS (RPVS) IN NUCLEAR POWER PLANTS SE Woodhead Publishing Series in Energy LA English DT Article; Book Chapter DE reactor pressure vessel (RPV) design; reactor pressure vessel (RPV) fabrication; ASME Code AB The general design following the American Society of Mechanical Engineers (ASME) Boiler and Pressure Vessel Code and fabrication processes used in the USA for nuclear reactor pressure vessels (RPVs) are described. Also, several RPVs in countries other than the USA were designed and fabricated in the USA using the processes described here. Detailed knowledge of the design and fabrication information is necessary to assure long-term structural integrity and safe operation of the RPVs. C1 [Server, W. L.] ATI Consulting, Black Mt, NC 28711 USA. [Nanstad, R. K.] Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37831 USA. RP Server, WL (reprint author), ATI Consulting, 6 Laurel Branch Dr,POB 879, Black Mt, NC 28711 USA. EM williamser@aol.com; nanstadrk@ornl.gov NR 4 TC 1 Z9 1 U1 1 U2 4 PU WOODHEAD PUBL LTD PI CAMBRIDGE PA ABINGTON HALL ABINGTON, CAMBRIDGE CB1 6AH, CAMBS, ENGLAND SN 2044-9364 BN 978-0-85709-647-0; 978-1-84569-967-3 J9 WOODHEAD PUBL SER EN PY 2015 IS 26 BP 3 EP 25 DI 10.1533/9780857096470.1.3 PG 23 WC Materials Science, Multidisciplinary; Nuclear Science & Technology SC Materials Science; Nuclear Science & Technology GA BC0EG UT WOS:000348986000002 ER PT S AU Server, WL Nanstad, RK AF Server, W. L. Nanstad, R. K. BE Soneda, N TI Integrity and embrittlement management of reactor pressure vessels (RPVs) in light-water reactors SO IRRADIATION EMBRITTLEMENT OF REACTOR PRESSURE VESSELS (RPVS) IN NUCLEAR POWER PLANTS SE Woodhead Publishing Series in Energy LA English DT Article; Book Chapter DE radiation embrittlement; pressurized thermal shock; fracture toughness; pressure-temperature limit curves; structural integrity AB Validation of the current and continued integrity approaches for the reactor pressure vessel (RPV) has been shown through the many years of safe operation of light-water reactor vessels. There have not been any vessel failures, and this fact is primarily due to proper embrittlement management programs and structural integrity assessment methods. Additionally, there have been several large-scale experiments performed to further validate the integrity of RPVs. This chapter is focused on the embrittlement and integrity management approaches used in different countries that are operating nuclear power plants. C1 [Server, W. L.] ATI Consulting, Black Mt, NC 28711 USA. [Nanstad, R. K.] Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37831 USA. RP Server, WL (reprint author), ATI Consulting, 6 Laurel Branch Dr,POB 879, Black Mt, NC 28711 USA. EM williamser@aol.com; nanstadrk@ornl.gov NR 29 TC 0 Z9 0 U1 0 U2 1 PU WOODHEAD PUBL LTD PI CAMBRIDGE PA ABINGTON HALL ABINGTON, CAMBRIDGE CB1 6AH, CAMBS, ENGLAND SN 2044-9364 BN 978-0-85709-647-0; 978-1-84569-967-3 J9 WOODHEAD PUBL SER EN PY 2015 IS 26 BP 132 EP 155 DI 10.1533/9780857096470.2.132 PG 24 WC Materials Science, Multidisciplinary; Nuclear Science & Technology SC Materials Science; Nuclear Science & Technology GA BC0EG UT WOS:000348986000007 ER PT S AU Nanstad, RK Server, WL Sokolov, MA Brumovsky, M AF Nanstad, R. K. Server, W. L. Sokolov, M. A. Brumovsky, M. BE Soneda, N TI Evaluating the fracture toughness of reactor pressure vessel (RPV) materials subject to embrittlement SO IRRADIATION EMBRITTLEMENT OF REACTOR PRESSURE VESSELS (RPVS) IN NUCLEAR POWER PLANTS SE Woodhead Publishing Series in Energy LA English DT Article; Book Chapter DE fracture toughness; J-integral; master curve; irradiation; crack-arrest; embrittlement; Charpy impact; nil-ductility transition (NDT) temperature; pressurized water reactor (PWR) ID MASTER CURVE ANALYSIS; FERRITIC STEELS; RADIATION; SPECIMENS; CHARPY AB This chapter discusses the fracture toughness of reactor pressure vessel (RPV) materials as a consequence of service in a neutron irradiation environment. Fracture toughness of the materials is directly related to structural integrity of the operating RPV and the materials must be evaluated relative to their radiation sensitivity and effects on overall structural integrity. In radiation-sensitive steel, the fracture toughness is decreased and is the property used to describe the radiation-induced embrittlement. The chapter presents a brief history of the development of fracture mechanics followed by more detailed discussions of different aspects of material fracture toughness under both quasi-static and dynamic loading conditions. C1 [Nanstad, R. K.; Sokolov, M. A.] Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37831 USA. [Server, W. L.] ATI Consulting, Black Mt, NC 28711 USA. [Brumovsky, M.] Nucl Res Inst Rez Plc, Husinec Rez 25068, Czech Republic. RP Nanstad, RK (reprint author), Oak Ridge Natl Lab, Mat Sci & Technol Div, 1 Bethel Valley Rd,MS 6138, Oak Ridge, TN 37831 USA. EM nanstadrk@ornl.gov; williamser@aol.com; sokolovm@ornl.gov; bru@ujv.cz NR 74 TC 0 Z9 0 U1 0 U2 1 PU WOODHEAD PUBL LTD PI CAMBRIDGE PA ABINGTON HALL ABINGTON, CAMBRIDGE CB1 6AH, CAMBS, ENGLAND SN 2044-9364 BN 978-0-85709-647-0; 978-1-84569-967-3 J9 WOODHEAD PUBL SER EN PY 2015 IS 26 BP 295 EP 332 DI 10.1533/9780857096470.3.295 PG 38 WC Materials Science, Multidisciplinary; Nuclear Science & Technology SC Materials Science; Nuclear Science & Technology GA BC0EG UT WOS:000348986000011 ER PT J AU Williams, PT AF Williams, Paul T. TI Lower Risk of Alzheimer's Disease Mortality with Exercise, Statin, and Fruit Intake SO JOURNAL OF ALZHEIMERS DISEASE LA English DT Article DE Alzheimer's disease; diet; epidemiology; prevention; prospective cohort study; running; statins; walking ID CORONARY-HEART-DISEASE; MILD COGNITIVE IMPAIRMENT; CLINICAL-TRIAL COHORT; MEDITERRANEAN DIET; PHYSICAL-ACTIVITY; VEGETABLE CONSUMPTION; REDUCED RISK; VITAMIN-D; DEMENTIA; CHOLESTEROL AB Background: Whether lifestyle affects Alzheimer's disease (AD) risk remains controversial. Objective: Test whether exercise, diet, or statins affect AD mortality in 153,536 participants of the National Runners' and Walkers' Health Studies. Methods: Hazard ratios (HR) and 95% confidence intervals (95% CI) were obtained from Cox proportional hazard analyses for AD mortality versus baseline metabolic equivalent (MET) hours/d of exercise energy expenditure (1 MET equals approximately 1 km run), statin use, and fruit intake when adjusted for age, race, gender, education, and exercise mode. Results: The National Death Index identified 175 subjects who died with AD listed as an underlying (n = 116) or contributing (n = 59) cause of death during 11.6-year average mortality surveillance. Relative to exercising <1.07 MET-hours/d, AD mortality was 6.0% lower for 1.07 to 1.8 MET-hours/d (HR: 0.94, 95% CI: 0.59 to 1.46, p = 0.79), 24.8% lower for 1.8 to 3.6 MET-hours/d (HR: 0.75, 95% CI: 0.50 to 1.13, p = 0.17), and 40.1% lower for >= 3.6 MET-hours/d (HR: 0.60, 95% CI: 0.37 to 0.97, p = 0.04). Relative to non-use, statin use was associated with 61% lower AD mortality (HR: 0.39, 95% CI: 0.15 to 0.82, p = 0.01), whereas use of other cholesterol-lowering medications was not (HR: 0.78, 95% CI: 0.40 to 1.38, p = 0.42). Relative to <1 piece of fruit/day, consuming 2 to 3 pieces daily was associated with 39.7% lower AD mortality (HR: 0.60, 95% CI: 0.39 to 0.91, p = 0.02) and >= 3 pieces/day with 60.7% lower AD mortality (HR: 0.39, 95% CI: 0.22 to 0.67, p = 0.0004). Conclusions: Exercise, statin, and fruit intake were associated with lower risk for AD mortality. C1 Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Life Sci, Berkeley, CA 94720 USA. RP Williams, PT (reprint author), Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Life Sci, Donner 464,1 Cyclotron Rd, Berkeley, CA 94720 USA. EM ptwilliams@lbl.gov FU National Heart, Lung, and Blood Institute [HL094717] FX This research was supported by grant HL094717 from the National Heart, Lung, and Blood Institute and was conducted at the Ernest Orlando Lawrence Berkeley National Laboratory (Department of Energy DE-AC03-76SF00098 to the University of California). The funders had no role in study design, data collection and analysis, decision to publish, or preparation of the manuscript. The authors have declared that no competing interests exist. PTW had full access to all of the data in the study and takes responsibility for the integrity of the data and the accuracy of the data analysis. NR 53 TC 9 Z9 9 U1 5 U2 20 PU IOS PRESS PI AMSTERDAM PA NIEUWE HEMWEG 6B, 1013 BG AMSTERDAM, NETHERLANDS SN 1387-2877 EI 1875-8908 J9 J ALZHEIMERS DIS JI J. Alzheimers Dis. PY 2015 VL 44 IS 4 BP 1121 EP 1129 DI 10.3233/JAD-141929 PG 9 WC Neurosciences SC Neurosciences & Neurology GA CC0BW UT WOS:000350001000008 PM 25408208 ER PT J AU Bridges, JC Schwenzer, SP Leveille, R Westall, F Wiens, RC Mangold, N Bristow, T Edwards, P Berger, G AF Bridges, J. C. Schwenzer, S. P. Leveille, R. Westall, F. Wiens, R. C. Mangold, N. Bristow, T. Edwards, P. Berger, G. TI Diagenesis and clay mineral formation at Gale Crater, Mars SO JOURNAL OF GEOPHYSICAL RESEARCH-PLANETS LA English DT Article DE Mars; Mars Science Laboratory; clay; Yellowknife Bay; diagenesis ID GENERATED HYDROTHERMAL SYSTEMS; ALTERATION ASSEMBLAGES; MARTIAN METEORITES; SATURATION STATE; YELLOWKNIFE BAY; NATURAL-WATERS; ORIGIN; DISSOLUTION; EVOLUTION; PHYLLOSILICATES AB The Mars Science Laboratory rover Curiosity found host rocks of basaltic composition and alteration assemblages containing clay minerals at Yellowknife Bay, Gale Crater. On the basis of the observed host rock and alteration minerals, we present results of equilibrium thermochemical modeling of the Sheepbed mudstones of Yellowknife Bay in order to constrain the formation conditions of its secondary mineral assemblage. Building on conclusions from sedimentary observations by the Mars Science Laboratory team, we assume diagenetic, in situ alteration. The modeling shows that the mineral assemblage formed by the reaction of a CO2-poor and oxidizing, dilute aqueous solution (Gale Portage Water) in an open system with the Fe-rich basaltic-composition sedimentary rocks at 10-50 degrees C and water/rock ratio (mass of rock reacted with the starting fluid) of 100-1000, pH of similar to 7.5-12. Model alteration assemblages predominantly contain phyllosilicates (Fe-smectite, chlorite), the bulk composition of a mixture of which is close to that of saponite inferred from Chemistry and Mineralogy data and to that of saponite observed in the nakhlite Martian meteorites and terrestrial analogues. To match the observed clay mineral chemistry, inhomogeneous dissolution dominated by the amorphous phase and olivine is required. We therefore deduce a dissolving composition of approximately 70% amorphous material, with 20% olivine, and 10% whole rock component. C1 [Bridges, J. C.; Edwards, P.] Univ Leicester, Dept Phys & Astron, Space Res Ctr, Leicester LE1 7RH, Leics, England. [Schwenzer, S. P.] Open Univ, Dept Phys Sci, Milton Keynes MK7 6AA, Bucks, England. [Leveille, R.] McGill Univ, Dept Earth & Planetary Sci, Montreal, PQ, Canada. [Westall, F.] CNRS, Ctr Biophys Mol, Orleans 2, France. [Wiens, R. C.] Los Alamos Natl Lab, Los Alamos, NM USA. [Mangold, N.] CNRS, UMR6112, LPGN, Nantes, France. [Mangold, N.] Univ Nantes, Nantes, France. [Bristow, T.] NASA, Ames Res Ctr, Exobiol Branch, Moffett Field, CA 94035 USA. [Berger, G.] Univ Toulouse 3, IRAP, CNRS, F-31062 Toulouse, France. RP Bridges, JC (reprint author), Univ Leicester, Dept Phys & Astron, Space Res Ctr, Leicester LE1 7RH, Leics, England. EM j.bridges@le.ac.uk RI BERGER, Gilles/F-7118-2016; OI Schwenzer, Susanne Petra/0000-0002-9608-0759 FU UKSA; OU Research Investment Fellowship FX J.C.B. and S.P.S. are funded by UKSA. S.P.S. was in part funded by an OU Research Investment Fellowship. The mineralogical data used for modeling from the Mars Science Laboratory mission in this paper are available in published articles, referred to in the text [e.g., Vaniman et al., 2014]. NR 59 TC 12 Z9 12 U1 3 U2 22 PU AMER GEOPHYSICAL UNION PI WASHINGTON PA 2000 FLORIDA AVE NW, WASHINGTON, DC 20009 USA SN 2169-9097 EI 2169-9100 J9 J GEOPHYS RES-PLANET JI J. Geophys. Res.-Planets PD JAN PY 2015 VL 120 IS 1 BP 1 EP 19 DI 10.1002/2014JE004757 PG 19 WC Geochemistry & Geophysics SC Geochemistry & Geophysics GA CC0WD UT WOS:000350058500001 ER PT J AU Kellerman, AC Shprits, YY Makarevich, RA Spanswick, E Donovan, E Reeves, G AF Kellerman, A. C. Shprits, Y. Y. Makarevich, R. A. Spanswick, E. Donovan, E. Reeves, G. TI Characterization of the energy-dependent response of riometer absorption SO JOURNAL OF GEOPHYSICAL RESEARCH-SPACE PHYSICS LA English DT Article DE cosmic noise absorption; riometer; electron precipitation; radiation belts; particle modeling; electron energy ID AURORAL RADIO ABSORPTION; RADIATION BELT ELECTRONS; IMAGING RIOMETER; RELATIVISTIC ELECTRONS; MORNING SECTOR; IONOSPHERIC ABSORPTION; RESONANT DIFFUSION; SPIKE EVENTS; COSMIC NOISE; E-REGION AB Ground-based riometers provide an inexpensive means to continuously remote sense the precipitation of electrons in the dynamic auroral region of Earth's ionosphere. The energy-dependent relationship between riometer absorption and precipitating electrons is thus of great importance for understanding the loss of electrons from the Earth's magnetosphere. In this study, statistical and event-based analyses are applied to determine the energy of electrons to which riometers chiefly respond. Time-lagged correlation analysis of trapped to precipitating fluxes shows that daily averaged absorption best correlates with approximate to 60 keV trapped electron flux at zero-time lag, although large variability is observed across different phases of the solar cycle. High-time resolution statistical cross-correlation analysis between signatures observed by riometer stations, and assuming electron motion due to gradient and curvature drift, results in inferred energies of 10-100 keV, with a clear maximum in occurrence for 40-60 keV electrons. One event is considered in detail utilizing riometer absorption signatures obtained from several stations. The mean inferred energies for the initial rise time and peak of the absorption after correction for electric field effects were approximate to 70 keV and approximate to 60 keV, respectively. The analyses presented provide a means to characterize the energy of electrons to which riometers are responding in both a statistical sense and during the evolution of individual events. C1 [Kellerman, A. C.; Shprits, Y. Y.] Univ Calif Los Angeles, Dept Earth Planetary & Space Sci, Los Angeles, CA 90095 USA. [Shprits, Y. Y.] MIT, Dept Earth Atmospher & Planetary Sci, Cambridge, MA 02139 USA. [Shprits, Y. Y.] Skolkovo Inst Sci & Technol, Skolkovo, Moscow Region, Russia. [Makarevich, R. A.] Univ Alaska Fairbanks, Inst Geophys, Fairbanks, AK 99775 USA. [Makarevich, R. A.] Univ Alaska Fairbanks, Dept Phys, Fairbanks, AK USA. [Spanswick, E.; Donovan, E.] Univ Calgary, Dept Phys & Astron, Calgary, AB T2N 1N4, Canada. [Reeves, G.] Los Alamos Natl Lab, Space Sci & Applicat Grp, Los Alamos, NM USA. RP Kellerman, AC (reprint author), Univ Calif Los Angeles, Dept Earth Planetary & Space Sci, Los Angeles, CA 90095 USA. EM akellerman@igpp.ucla.edu RI Kellerman, Adam/B-6525-2013; Reeves, Geoffrey/E-8101-2011; OI Kellerman, Adam/0000-0002-2315-936X; Reeves, Geoffrey/0000-0002-7985-8098; Donovan, Eric/0000-0002-8557-4155 FU NSF CEDAR [AGS-1243183]; UC Lab Fees Research Program [116720] FX This research was supported by NSF CEDAR grant AGS-1243183 and UC Lab Fees Research Program grant 116720. The authors would like to thank Reeves et al. [2011] for providing the long-term daily averaged LANL/GEO data set. The OMNI data are available at ftp://nssdcftp.gsfc.nasa.gov/spacecraft_data/omni/omni2.txt, the riometer data are available at ftp://aurora.phys.ucalgary.ca/data/riometer/. This work used computational and storage services associated with the Hoffman2 Shared Cluster provided by UCLA Institute for Digital Research and Education's Research Technology Group. NR 77 TC 1 Z9 1 U1 0 U2 2 PU AMER GEOPHYSICAL UNION PI WASHINGTON PA 2000 FLORIDA AVE NW, WASHINGTON, DC 20009 USA SN 2169-9380 EI 2169-9402 J9 J GEOPHYS RES-SPACE JI J. Geophys. Res-Space Phys. PD JAN PY 2015 VL 120 IS 1 BP 615 EP 631 DI 10.1002/2014JA020027 PG 17 WC Astronomy & Astrophysics SC Astronomy & Astrophysics GA CB8OX UT WOS:000349891300040 ER PT J AU Venna, SR Lartey, M Li, T Spore, A Kumar, S Nulwala, HB Luebke, DR Rosi, NL Albenze, E AF Venna, Surendar R. Lartey, Michael Li, Tao Spore, Alex Kumar, Santosh Nulwala, Hunaid B. Luebke, David R. Rosi, Nathaniel L. Albenze, Erik TI Fabrication of MMMs with improved gas separation properties using externally-functionalized MOF particles SO JOURNAL OF MATERIALS CHEMISTRY A LA English DT Article ID MIXED-MATRIX MEMBRANES; METAL-ORGANIC FRAMEWORKS; CO2/CH4 SEPARATION; GLASSY-POLYMERS; PORE-SIZE; ZEOLITE; NANO; PERFORMANCE; COMPOSITES; ADSORPTION AB Mixed matrix membranes (MMM) have the potential to overcome the limitations of traditional polymeric membranes for gas separation by improving both the permeability and selectivity. The most difficult challenge is accessing defect free and optimized MMM membranes. Defects are generally due to incompatible interfaces between the polymer and the filler particle. Herein, we present a new approach to modify and optimize the surface of UiO-66-NH2 based MOF particles to improve its interaction with Matrimid (R) polymer. A series of surface modified UiO-66-NH2 particles were synthesized and characterized using H-1 NMR spectroscopy, mass spectrometry, XPS, and powder X-ray diffraction. MMMs containing surface optimized MOF particles exhibit improved thermal and mechanical properties. Most importantly, the MMMs show significantly enhanced gas separation properties; CO2 permeability was increased by similar to 200% and CO2/N-2 ideal selectivity was increased by similar to 25%. These results confirm the success of the proposed technique to mitigate defective MOF/Matrimid (R) interfaces. C1 [Venna, Surendar R.; Lartey, Michael; Kumar, Santosh; Nulwala, Hunaid B.; Luebke, David R.; Albenze, Erik] Natl Energy Technol Lab, Pittsburgh, PA 15236 USA. [Venna, Surendar R.] W Virginia Univ, Corp Res, Morgantown, WV 26506 USA. [Li, Tao; Spore, Alex; Rosi, Nathaniel L.] Univ Pittsburgh, Pittsburgh, PA 15260 USA. [Nulwala, Hunaid B.] Carnegie Mellon Univ, Pittsburgh, PA 15213 USA. [Albenze, Erik] URS Energy & Construct, Pittsburgh, PA 15236 USA. [Lartey, Michael; Kumar, Santosh] Oak Ridge Inst Sci & Educ, Oak Ridge, TN 37831 USA. RP Albenze, E (reprint author), Natl Energy Technol Lab, Pittsburgh, PA 15236 USA. EM nrosi@pitt.edu; erik.albenze@netl.doe.gov OI Nulwala, Hunaid/0000-0001-7481-3723 FU National Energy Technology Laboratory's ongoing research under the RES [DE-FE0004000] FX This technical effort was performed in support of the National Energy Technology Laboratory's ongoing research under the RES contract DE-FE0004000. The authors would like to thank Dr Brian Adzima and Dr Elliot Roth for their input in thermal analysis of membrane using DSC. NR 50 TC 26 Z9 26 U1 26 U2 119 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7488 EI 2050-7496 J9 J MATER CHEM A JI J. Mater. Chem. A PY 2015 VL 3 IS 9 BP 5014 EP 5022 DI 10.1039/c4ta05225k PG 9 WC Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary SC Chemistry; Energy & Fuels; Materials Science GA CC0AM UT WOS:000349997000033 ER PT J AU Lv, LF Chen, Z Liu, GK Huang, SM Pan, YX AF Lv, Lifen Chen, Zhen Liu, Guokui Huang, Shaoming Pan, Yuexiao TI Optimized photoluminescence of red phosphor K2TiF6:Mn4+ synthesized at room temperature and its formation mechanism SO JOURNAL OF MATERIALS CHEMISTRY C LA English DT Article ID LIGHT-EMITTING-DIODES; OPTICAL-PROPERTIES; HF/KMNO4 SOLUTION; LED APPLICATIONS; LUMINESCENCE AB A red phosphor K2TiF6:Mn4+ (KTFM) has been synthesized by etching Ti(OC4H9)(4) in HF solution with KMnO4 and KF at room temperature for 30 min. The formation mechanism of red phosphor KTFM has been discussed based on detailed experimental results. We studied the influences of synthetic procedure and KMnO4 concentration on the powder color and intensity of phosphor luminescence. The actual doping concentration of Mn4+ in the K2TiF6 (KTF) host lattice of the phosphor has been investigated by measuring the concentration of filtrate through ICP-AES analysis. The results showed that about 32.4 mol% of Mn elements was doped into KTF crystals at optimal Mn4+ concentration (in precursor solution). The presence of HF was found to be essential to doping Mn4+ into KTF due to the weakly acidic and complexing properties of HF. The red luminescence of Mn4+ in KTF with a crystal structure matching standard card JCPDs (#28-0825), was first observed in the sample prepared from HF solution concentrations lower than 5 wt%. The dependence of the intensity of the luminescence on HF concentration might be due to the varying of Mn4+ concentrations in KTF crystals. Higher HF concentration was associated with lower yield, because KTF is soluble in HF at high concentrations. Encapsulation of the red phosphor KTFM with YAG:Ce on a GaN layer produces "warm" white LEDs with color rendering of 86 at 3251 K. C1 [Lv, Lifen; Chen, Zhen; Huang, Shaoming; Pan, Yuexiao] Wenzhou Univ, Fac Chem & Mat Engn, Nanomat & Chem Key Lab, Wenzhou 325027, Zhejiang, Peoples R China. [Liu, Guokui] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. RP Pan, YX (reprint author), Wenzhou Univ, Fac Chem & Mat Engn, Nanomat & Chem Key Lab, Wenzhou 325027, Zhejiang, Peoples R China. EM yxpan8@gmail.com FU Chinese NSF [51102185]; Qianjiang Talents Project [R20131019] FX This research was jointly supported by Chinese NSF (Grant no. 51102185) and Qianjiang Talents Project (Grant no. R20131019). NR 36 TC 26 Z9 26 U1 7 U2 63 PU ROYAL SOC CHEMISTRY PI CAMBRIDGE PA THOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND SN 2050-7526 EI 2050-7534 J9 J MATER CHEM C JI J. Mater. Chem. C PY 2015 VL 3 IS 9 BP 1935 EP 1941 DI 10.1039/c4tc02097a PG 7 WC Materials Science, Multidisciplinary; Physics, Applied SC Materials Science; Physics GA CB6TG UT WOS:000349759000008 ER PT J AU Borodin, O Han, SD Daubert, JS Seo, DM Yun, SH Henderson, WA AF Borodin, Oleg Han, Sang-Don Daubert, James S. Seo, Daniel M. Yun, Sung-Hyun Henderson, Wesley A. TI Electrolyte Solvation and Ionic Association VI. Acetonitrile-Lithium Salt Mixtures: Highly Associated Salts Revisited SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID N,N'-AROMATIC BIDENTATE LIGANDS; MOLECULAR-DYNAMICS SIMULATIONS; AMORPHOUS CONCENTRATED LIQUID; LI+ CATION COORDINATION; POLYMER ELECTROLYTES; CRYSTAL-STRUCTURES; LOCAL STRUCTURES; GROUP-1 SALTS; BASE RATIO; COMPLEXES AB Molecular dynamics (MD) simulations of acetonitrile (AN) mixtures with LiBF4, LiCF3SO3 and LiCF3CO2 provide extensive details about the molecular- and mesoscale-level solution interactions and thus explanations as to why these electrolytes have very different thermal phase behavior and electrochemical/physicochemical properties. The simulation results are in full accord with a previous experimental study of these (AN)(n)-LiX electrolytes. This computational study reveals how the structure of the anions strongly influences the ionic association tendency of the ions, the manner in which the aggregate solvates assemble in solution and the length of time in which the anions remain coordinated to the Li+ cations in the solvates which result in dramatic variations in the transport properties of the electrolytes. (C) The Author(s) 2015. Published by ECS. This is an open access article distributed under the terms of the Creative Commons Attribution 4.0 License (CC BY, http://creativecommons.org/licenses/by/4.0/), which permits unrestricted reuse of the work in any medium, provided the original work is properly cited. All rights reserved. C1 [Borodin, Oleg] US Army Res Lab, Electrochem Branch, Adelphi, MD 20783 USA. [Han, Sang-Don; Daubert, James S.; Seo, Daniel M.; Henderson, Wesley A.] N Carolina State Univ, Dept Chem & Biomol Engn, Ion Liquids & Electrolytes Energy Technol ILEET L, Raleigh, NC 27695 USA. [Yun, Sung-Hyun] Gwangju Inst Sci & Technol, Sch Environm Sci & Engn, Kwangju 500712, South Korea. [Henderson, Wesley A.] Pacific NW Natl Lab, Energy & Environm Directorate, Electrochem Mat & Syst EMS Grp, Richland, WA 99352 USA. RP Borodin, O (reprint author), US Army Res Lab, Electrochem Branch, Adelphi, MD 20783 USA. EM oleg.a.borodin.civ@mail.mil; Wesley.Henderson@pnnl.gov RI Borodin, Oleg/B-6855-2012; OI Borodin, Oleg/0000-0002-9428-5291; Daubert, James/0000-0002-8151-9191 FU Department of Energy [DE-IA01-11EE003413]; U.S. Army Research Laboratory [DE-IA01-11EE003413]; U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering [DE-SC0002169] FX The computational work was partially supported by an Interagency Agreement between the U.S. Department of Energy and the U.S. Army Research Laboratory under DE-IA01-11EE003413 for the Office of Vehicle Technologies Programs including the Batteries for Advanced Transportation Technologies (BATT) Program. The authors wish to also express their gratitude to the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering which supported the evaluation of the computational work and preparation of the manuscript under Award DE-SC0002169. NR 41 TC 8 Z9 8 U1 3 U2 32 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 EI 1945-7111 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2015 VL 162 IS 4 BP A501 EP A510 DI 10.1149/2.0891503jes PG 10 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA CB7SG UT WOS:000349827200002 ER PT J AU Dees, DW Abraham, DP Lu, WQ Gallagher, KG Bettge, M Jansen, AN AF Dees, Dennis W. Abraham, Daniel P. Lu, Wenquan Gallagher, Kevin G. Bettge, Martin Jansen, Andrew N. TI Electrochemical Modeling and Performance of a Lithium- and Manganese-Rich Layered Transition-Metal Oxide Positive Electrode SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID ION BATTERIES; POROUS-ELECTRODE; CATHODE PERFORMANCE; COMPOSITE CATHODES; INSERTION CELL; VOLTAGE FADE; IMPEDANCE; OPTIMIZATION; CONDUCTIVITY; HYSTERESIS AB The impedance of a lithium- and manganese-rich layered transition-metal oxide (MR-NMC) positive electrode, specifically Li1.2Ni0.15Mn0.55Co0.1O2, is compared to two other transition-metal layered oxide materials, specifically LiNi0.8Co0.15Al0.05O2 (NCA) and Li-1.05(Ni1/3Co1/3Mn1/3)(0.95)O-2 (NMC). A more detailed electrochemical impedance spectroscopy (EIS) study is conducted on the LMR-NMC electrode, which includes a range of states-of-charge (SOCs) for both current directions (i.e. charge and discharge) and two relaxation times (i.e. hours and one hundred hours) before the EIS sweep. The LMR-NMC electrode EIS studies are supported by half-cell constant current and galvanostatic intermittent titration technique (GITT) studies. Two types of electrochemical models are utilized to examine the results. The first type is a lithium ion cell electrochemical model for intercalation active material electrodes that includes a complex active material/electrolyte interfacial structure. The other is a lithium ion half-cell electrochemical model that focuses on the unique composite structure of the bulk LMR-NMC materials. (C) 2015 The Electrochemical Society. All rights reserved. C1 [Dees, Dennis W.; Abraham, Daniel P.; Lu, Wenquan; Gallagher, Kevin G.; Bettge, Martin; Jansen, Andrew N.] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. RP Dees, DW (reprint author), Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM dees@anl.gov RI Jansen, Andrew/Q-5912-2016 OI Jansen, Andrew/0000-0003-3244-7790 FU U.S. Department of Energy Office of Science laboratory [DE-AC02-06CH11357] FX Support from the Vehicle Technologies Program, Hybrid and Electric Systems, David Howell (Team Lead) and Peter Faguy, at the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, is gratefully acknowledged. The submitted manuscript has been created by UChicago Argonne, LLC, Operator of Argonne National Laboratory ("Argonne"). Argonne, a U.S. Department of Energy Office of Science laboratory, is operated under Contract No. DE-AC02-06CH11357. The U.S. Government retains for itself, and others acting on its behalf, a paid-up nonexclusive, irrevocable worldwide license in said article to reproduce, prepare derivative works, distribute copies to the public, and perform publicly and display publicly, by or on behalf of the Government. NR 44 TC 5 Z9 5 U1 9 U2 85 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 EI 1945-7111 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2015 VL 162 IS 4 BP A559 EP A572 DI 10.1149/2.0231504jes PG 14 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA CB7SG UT WOS:000349827200010 ER PT J AU Deshpande, RD Ridgway, P Fu, YB Zhang, W Cai, JS Battaglia, V AF Deshpande, Rutooj D. Ridgway, Paul Fu, Yanbao Zhang, Wei Cai, Jinshu Battaglia, Vincent TI The Limited Effect of VC in Graphite/NMC Cells SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID LI-ION BATTERIES; SURFACE-FILM FORMATION; VINYLENE CARBONATE; NEGATIVE ELECTRODE; FORMING ADDITIVES; CYCLE LIFE; PERFORMANCE; SPECTROSCOPY; TEMPERATURE AB Degradation at the electrode surfaces is one of the major reasons behind capacity fade in well-constructed batteries. The effect of electrolyte additives, in particular vinylene carbonate (VC), is studied extensively for different lithium-ion chemistries and is shown to improve columbic efficiency of some electrodes. We investigate the effect of VC additive in a graphite/NMC333 (lithiumnickel-manganese-cobalt oxide) cell. The addition of VC improves the rate performance, especially, at moderately high rates. A new three-electrode cell design with Li reference electrode was particularly useful in studying the rate performance of each electrode. The rate of side reactions is found to decrease with the addition of VC. Despite these important performance improvements, no significant improvement in the capacity retention is observed. This suggests that the side reactions in graphite/NCM cells consist of two types, (1) repairing cracked solid electrolyte interphase (SEI) on the negative electrode (results in a net consumption of Li from the positive electrode), (2) reforming SEI components that dissolve from the negative electrode and are oxidized at the positive electrode. The VC appears to reduce the second type but have negligible effect on the first. This indicates that columbic efficiency measurements are not a reliable indicator of cell cycle life. (C) The Author(s) 2014. Published by ECS. All rights reserved. C1 [Deshpande, Rutooj D.] Ford Motor Co, Electrified Powertrain Engn, Detroit, MI 48124 USA. [Ridgway, Paul; Fu, Yanbao; Zhang, Wei; Cai, Jinshu; Battaglia, Vincent] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Energy & Environm Technol Div, Berkeley, CA 94720 USA. RP Deshpande, RD (reprint author), Ford Motor Co, Electrified Powertrain Engn, Detroit, MI 48124 USA. EM rdeshpan@ford.com RI Fu, Yanbao/F-9583-2011 OI Fu, Yanbao/0000-0001-7752-680X FU BATT program; U.S. Department of Energy FX The authors acknowledge the BATT program and the U.S. Department of Energy for funding this project. NR 22 TC 8 Z9 8 U1 6 U2 43 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 EI 1945-7111 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2015 VL 162 IS 3 BP A330 EP A338 DI 10.1149/2.0221503jes PG 9 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA CB7QZ UT WOS:000349823700013 ER PT J AU Hudak, NS Davis, LE Nagasubramanian, G AF Hudak, Nicholas S. Davis, Lorie E. Nagasubramanian, Ganesan TI Cycling-Induced Changes in the Entropy Profiles of Lithium Cobalt Oxide Electrodes SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID MONTE-CARLO SIMULATION; X-RAY-DIFFRACTION; LI-ION BATTERIES; MANGANESE OXIDE; CAPACITY FADE; INTERCALATION; THERMODYNAMICS; GRAPHITE; CHARGE; DISCHARGE AB Entropy profiles of lithium cobalt oxide (LiCoO2) electrodes were measured at various stages in their cycle life to examine performance degradation and cycling-induced changes, or lack thereof, in thermodynamics. LiCoO2 electrodes were cycled at C/2 rate in half-cells (vs. lithium anodes) up to 20 cycles or C/5 rate in full cells (vs. MCMB anodes) up to 500 cycles. The electrodes were then subjected to entropy measurements (partial derivative E/partial derivative T, where E is open-circuit potential and T is temperature) in half-cells at regular intervals over the approximate range 0.5 <= x <= 1 in LixCoO2. Despite significant losses in capacity, the cycling did not result in any change to the overall shape of the entropy profile, indicating retention of the LiCoO2 structure, lithium insertion mechanism, and thermodynamics. This confirms that cycling-induced performance degradation in LiCoO2 electrodes is primarily caused by kinetic barriers that increase with cycling. Electrodes cycled at C/5 exhibited a subtle, quantitative, and gradual change in the entropy profile in the narrow potential range of the hexagonal-to-monoclinic phase transition. The observed change is indicative of a decrease in the intralayer lithium ordering that occurs at these potentials, and it demonstrates that a cycling-induced structural disorder accompanies the kinetic degradation mechanisms. (C) The Author(s) 2014. Published by ECS. All rights reserved. C1 [Hudak, Nicholas S.; Davis, Lorie E.; Nagasubramanian, Ganesan] Sandia Natl Labs, Albuquerque, NM 87185 USA. RP Hudak, NS (reprint author), Sandia Natl Labs, POB 5800, Albuquerque, NM 87185 USA. EM nhudak@sandia.gov RI Hudak, Nicholas/D-3529-2011 FU Laboratory Directed Research and Development program at Sandia National Laboratories; U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000] FX The authors thank John Sullivan and Mark Rodriguez, both of Sandia National Laboratories, for helpful discussions. The authors gratefully acknowledge the financial support of the Laboratory Directed Research and Development program at Sandia National Laboratories. Sandia National Laboratories is a multiprogram laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000. NR 49 TC 2 Z9 2 U1 2 U2 17 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 EI 1945-7111 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2015 VL 162 IS 3 BP A315 EP A321 DI 10.1149/2.0071503jes PG 7 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA CB7QZ UT WOS:000349823700011 ER PT J AU Knehr, KW Eng, C Chen-Wiegart, YCK Wang, J West, AC AF Knehr, K. W. Eng, Christopher Chen-Wiegart, Yu-chen Karen Wang, Jun West, Alan C. TI In Situ Transmission X-Ray Microscopy of the Lead Sulfate Film Formation on Lead in Sulfuric Acid SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID ACTIVE-PASSIVE TRANSITION; EC-AFM; NEGATIVE ELECTRODES; ANODIC OXIDATION; FORM PBSO4; BATTERIES; PB; MECHANISM; PERFORMANCE; DISSOLUTION AB Transmission X-ray microscopy is utilized to monitor, in real time, the behavior of the PbSO4 film that is formed on Pb in H2SO4. Images collected from the synchrotron x-rays are coupled with voltammetric data to study the initial formation, the resulting passivation, and the subsequent reduction of the film. It is concluded with support from quartz-crystal-microbalance experiments that the initial formation of PbSO4 crystals occurs as a result of acidic corrosion. In addition, the film is shown to coalesce during the early stages of galvanostatic oxidation and to passivate as a result of morphological changes in the existing film. Finally, it is observed that the passivation process results in the formation of large PbSO4 crystals with low area-to-volume ratios, which are difficult to reduce under both galvanostatic and potentiostatic conditions. (C) The Author(s) 2014. Published by ECS. All rights reserved. C1 [Knehr, K. W.; West, Alan C.] Columbia Univ, Dept Chem Engn, New York, NY 10027 USA. [Eng, Christopher; Chen-Wiegart, Yu-chen Karen; Wang, Jun] Brookhaven Natl Lab, Photon Sci Directorate, Upton, NY 11973 USA. RP Knehr, KW (reprint author), Columbia Univ, Dept Chem Engn, New York, NY 10027 USA. EM kwk2111@columbia.edu RI Knehr, Kevin/R-4127-2016 OI Knehr, Kevin/0000-0001-5571-1537 FU National Science Foundation [1144155]; American Recovery and Reinvestment Act through 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-AC02-98CH10886] FX K. W. K. greatly acknowledges the support of the National Science Foundation Graduate Research Fellowship under grant No. 1144155. Any opinions, findings, and conclusions or recommendations expressed in this material are those of the authors and do not necessarily reflect the views of the National Science Foundation.; This work was supported in part by the American Recovery and Reinvestment Act funding through Department of Energy, Office of Science, Office of Basic Energy Sciences. Use of the National Synchrotron Light Source, Brookhaven National Laboratory for this work was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-98CH10886. NR 41 TC 2 Z9 2 U1 3 U2 18 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 EI 1945-7111 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2015 VL 162 IS 3 BP A255 EP A261 DI 10.1149/2.0141503jes PG 7 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA CB7QZ UT WOS:000349823700002 ER PT J AU Lee, E Koritala, R Miller, DJ Johnson, CS AF Lee, Eungje Koritala, Rachel Miller, Dean J. Johnson, Christopher S. TI Aluminum and Gallium Substitution into 0.5Li(2)MnO3 center dot 0.5Li(Ni0.375Mn0.375Co0.25)O-2 Layered Composite and the Voltage Fade Effect SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID LITHIUM-ION BATTERIES; X-RAY-DIFFRACTION; CATHODE MATERIALS; ELECTROCHEMICAL PERFORMANCE; LOCAL-STRUCTURE; SECONDARY BATTERIES; ELECTRON-MICROSCOPY; RECHARGEABLE CELLS; MANGANESE OXIDES; SPINEL PHASE AB Lithium- and manganese- rich layered composite cathodes in the general form (Li2MnO3 center dot LiMO2; M = transition metals), suffer from voltage profile suppression during cycling in Li- ion cells leading to overall gradual energy losses in the system. The suppression in cathode voltage which is called ` voltage fade' is a general phenomenon for these class of materials which needs to be understood and mitigated for enabling this chemistry in advanced Li- ion cells. Synthetic manipulation of the composition in 0.5Li(2)MnO(3)center dot 0.5LiNi(0.375)Mn(0.375)Co(0.25)O(2) (= Li1.2Ni0.15Mn0.55Co0.1O2 in layered notation) cathode material via aluminum and gallium substitution (max. 10%) via sol- gel reaction was completed and the voltage fade percentage was measured following a prescribed electrochemical testing protocol. While the specific capacities (similar to 250 mAh/g) are unaffected by the Al and Ga substitution (up to 5%), similar to 3 to 4% of the impedance- corrected average voltage is still lost (first 25 cycles) which is comparable to what the pristine material experiences. This result suggests that the path of structural change that occurs in the material during Li cycling is unaltered by synthetic manipulation of octahedral and/or tetrahedral sites though the use of Al and Ga non- redox active cations. (C) The Author(s) 2014. Published by ECS. All rights reserved. C1 [Lee, Eungje; Johnson, Christopher S.] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA. [Koritala, Rachel; Miller, Dean J.] Argonne Natl Lab, Electron Microscopy Ctr, Ctr Nanoscale Mat, Argonne, IL 60439 USA. RP Lee, E (reprint author), Argonne Natl Lab, Chem Sci & Engn Div, 9700 S Cass Ave, Argonne, IL 60439 USA. EM eungje.lee@anl.gov FU U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]; U.S. Department of Energy Office of Science [DE-AC02-06CH11357] FX Support from the Vehicle Technologies Program, Hybrid and Electric Systems, in particular, David Howell, Tien Duong, and Peter Faguy, at the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy is gratefully acknowledged. Use of the Center for Nanoscale Materials, including resources in the Electron Microscopy Center, was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, 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. NR 46 TC 17 Z9 17 U1 7 U2 56 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 EI 1945-7111 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2015 VL 162 IS 3 BP A322 EP A329 DI 10.1149/2.0321503jes PG 8 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA CB7QZ UT WOS:000349823700012 ER PT J AU Schauser, NS Harry, KJ Parkinson, DY Watanabe, H Balsara, NP AF Schauser, Nicole S. Harry, Katherine J. Parkinson, Dilworth Y. Watanabe, Hiroshi Balsara, Nitash P. TI Lithium Dendrite Growth in Glassy and Rubbery Nanostructured Block Copolymer Electrolytes SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID TIME-TEMPERATURE SUPERPOSITION; COMPOSITE POLYMER ELECTROLYTES; ALKALI-METAL SALTS; POLY(ETHYLENE OXIDE); MOLECULAR-WEIGHT; ELECTROCHEMICAL PROPERTIES; LITHIUM/POLYMER CELLS; MECHANICAL-PROPERTIES; ORGANIC ELECTROLYTE; IONIC-CONDUCTIVITY AB Enabling the use of lithium metal anodes is a critical step required to dramatically increase the energy density of rechargeable batteries. However, dendrite growth in lithium metal batteries, and a lack of fundamental understanding of the factors governing this growth, is a limiting factor preventing their adoption. Herein we present the effect of battery cycling temperature, ranging from 90 to 120 degrees C, on dendrite growth through a polystyrene-block-poly(ethylene oxide)-based electrolyte. This temperature range encompasses the glass transition temperature of polystyrene (107 degrees C). A slight increase in the cycling temperature of symmetric lithium-polymer-lithium cells from 90 to 105 degrees C results in a factor of five decrease in the amount of charge that can be passed before short circuit. Synchrotron hard X-ray microtomography experiments reveal a shift in dendrite location from primarily within the lithium electrode at 90 degrees C, to primarily within the electrolyte at 105 degrees C. Rheological measurements show a large change in mechanical properties over this temperature window. Time-temperature superposition was used to interpret the rheological data. Dendrite growth characteristics and cell lifetimes correlate with the temperature-dependent shift factors used for time-temperature superposition. Our work represents a step toward understanding the factors that govern lithium dendrite growth in viscoelastic electrolytes. (C) The Author(s) 2014. Published by ECS. All rights reserved. C1 [Schauser, Nicole S.; Harry, Katherine J.] Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. [Schauser, Nicole S.; Harry, Katherine J.; Balsara, Nitash P.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA. [Parkinson, Dilworth Y.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Adv Light Source Div, Berkeley, CA 94720 USA. [Watanabe, Hiroshi] Kyoto Univ, Inst Chem Res, Uji, Kyoto 6110011, Japan. [Balsara, Nitash P.] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. [Balsara, Nitash P.] Univ Calif Berkeley, Dept Chem & Biomol Engn, Berkeley, CA 94720 USA. RP Schauser, NS (reprint author), Univ Calif Berkeley, Dept Mat Sci & Engn, Berkeley, CA 94720 USA. EM nbalsara@berkeley.edu FU Electron Microscopy of Soft Matter Program from the Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division of the U.S. Department of Energy [DE-AC02-05CH11231]; BATT program from the Vehicle Technologies program, through the Office of Energy Efficiency and Renewable Energy under U.S. DOE [DE-AC02-05CH11231]; Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231]; National Science Foundation Graduate Research Fellowship FX We thank Jing Sun of the Lawrence Berkeley National Laboratory, for her help with the DSC sample preparation and measurements. Primary funding for the work was provided by the Electron Microscopy of Soft Matter Program from the 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 battery assembly portion of the project was supported by the BATT program from the Vehicle Technologies program, through the Office of Energy Efficiency and Renewable Energy under U.S. DOE Contract DE-AC02-05CH11231. Hard X-ray microtomography experiments were performed at the Advanced Light Source 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. Katherine J. Harry was supported by a National Science Foundation Graduate Research Fellowship. NR 67 TC 11 Z9 11 U1 13 U2 84 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 EI 1945-7111 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2015 VL 162 IS 3 BP A398 EP A405 DI 10.1149/2.0511503jes PG 8 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA CB7QZ UT WOS:000349823700022 ER PT J AU Takahashi, K Srinivasan, V AF Takahashi, Kenji Srinivasan, Venkat TI Examination of Graphite Particle Cracking as a Failure Mode in Lithium-Ion Batteries: A Model-Experimental Study SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID HYBRID-ELECTRIC VEHICLES; DIFFUSION-COEFFICIENT; RATE CAPABILITY; INDUCED STRESS; CAPACITY FADE; CELL; INTERCALATION; DEGRADATION; SIMULATION; FRACTURE AB Capacity fade in lithium-ion batteries remains an area of active research, with failure of the graphite anode thought to be an important contributor. While the formation of the solid electrolyte interphase and the subsequent loss of cyclable lithium have been well studied, mechanical degradation remains an area where ambiguity remains. While there appears to be little experimental evidence that suggest that macroscopic particle cracking occurs, mathematical models have suggested that this phenomenon is likely. The goal of this paper is to clarify this ambiguity by combining experimental cycling, mathematical stress modeling, and post-mortem microscopy. We experimentally determine an average diffusion coefficient of lithium in graphite using a thin-layer electrode and use this information in a diffusion-induced stress model. Our results suggest that cracking is not likely during lithiation due to the proximity of equilibrium potential to the cutoff potential. On delithiation, at 25 degrees C, even at 30 Crate cracking is unlikely while at -10 degrees C, a rate of 10 degrees C can lead to particle cracking. By extrapolating the results of the thin-layer electrode to a thick porous electrode, we found that graphite cracking is unlikely to occur during typical vehicle operations. (C) The Author(s) 2015. Published by ECS. This is an open access article distributed under the terms of the Creative Commons Attribution Non-Commercial No Derivatives 4.0 License (CC BY-NC-ND, http://creativecommons.org/licenses/by-nc-nd/4.0/), which permits non-commercial reuse, distribution, and reproduction in any medium, provided the original work is not changed in any way and is properly cited. For permission for commercial reuse, please email: oa@electrochem.org.All rights reserved. C1 [Takahashi, Kenji] Toyota Motor Co Ltd, Hybrid Vehicle Battery Unit, Dev Div, Toyota, Aichi 4718571, Japan. [Takahashi, Kenji; Srinivasan, Venkat] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Environm Energy Technol Div, Berkeley, CA 94720 USA. RP Takahashi, K (reprint author), Toyota Motor Co Ltd, Hybrid Vehicle Battery Unit, Dev Div, Toyota, Aichi 4718571, Japan. EM kenjitakahashi@mail.toyota.co.jp FU Office of Vehicle Technologies of the U.S. Department of Energy [DE-AC02-05CH11231] FX This work was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231 under the Batteries for Advanced Transportation Technologies (BATT) Program. NR 43 TC 15 Z9 15 U1 6 U2 43 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 EI 1945-7111 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2015 VL 162 IS 4 BP A635 EP A645 DI 10.1149/2.0281504jes PG 11 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA CB7SG UT WOS:000349827200019 ER PT J AU Takeuchi, ES Kim, YJ Huang, JP Marschilok, AC Takeuchi, KJ AF Takeuchi, Esther S. Kim, Young Jin Huang, Jianping Marschilok, Amy C. Takeuchi, Kenneth J. TI Electrochemistry of Cu0.5VOPO4 center dot 2H(2)O: A Promising Mixed Metal Phosphorous Oxide for Secondary Lithium based Batteries SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID X-RAY-DIFFRACTION; CATHODE MATERIAL; ABSORPTION SPECTROSCOPY; HYDROTHERMAL SYNTHESIS; MECHANISTIC INSIGHTS; ION BATTERIES; IN-SITU; PHOSPHATES; CUV2O6; LI AB Bimetallic mixed metal vanadium phosphorous oxide structures (MM'PxOy) have been the subject of much recent electrochemistry study. In analogy to silver vanadium phosphorous oxides, this study involves copper vanadium phosphorous oxide. Under galvanostatic discharge in lithium anode cells, the Cu0.5VOPO4 center dot 2H(2)O (CuVPO) material delivered similar to 280 mAh/g to 1.5 V. Unlike silver vanadium phosphorous oxides, crystallographic evaluation indicated little structural change upon electrochemical reduction of CuVPO, with no significant change in interlayer spacing and no evidence of copper metal formation. Notably, secondary battery evaluation showed retention of similar to 100 mAh/g at C/20 with little fade, a significant improvement under repeated cycling relative to a related silver based material. (C) The Author(s) 2014. Published by ECS. All rights reserved. C1 [Takeuchi, Esther S.; Huang, Jianping; Marschilok, Amy C.; Takeuchi, Kenneth J.] SUNY Stony Brook, Dept Chem, Stony Brook, NY 11790 USA. [Takeuchi, Esther S.; Marschilok, Amy C.; Takeuchi, Kenneth J.] SUNY Stony Brook, Dept Mat Sci & Engn, Stony Brook, NY 11790 USA. [Takeuchi, Esther S.] Brookhaven Natl Lab, Upton, NY 11973 USA. [Kim, Young Jin] SUNY Buffalo, Dept Chem & Biol Engn, Buffalo, NY 14260 USA. RP Takeuchi, ES (reprint author), SUNY Stony Brook, Dept Chem, Stony Brook, NY 11790 USA. EM esther.takeuchi@stonybrook.edu; amy.marschilok@stonybrook.edu; kenneth.takeuchi.1@stonybrook.edu RI Huang, Jianping/C-9379-2014 OI Huang, Jianping/0000-0002-8391-1381 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 The synthesis, characterization, study as a secondary battery material, and mechanistic investigation of the material as a function of electrochemical reduction were supported by the Department of Energy, Office of Basic Energy Sciences, under grant DE-SC0008512. Primary battery use studies evaluating pulse performance were supported by the National Institutes of Health under grant 1R01HL093044-01A1 from the National Heart, Lung, and Blood Institute. NR 31 TC 0 Z9 0 U1 3 U2 23 PU ELECTROCHEMICAL SOC INC PI PENNINGTON PA 65 SOUTH MAIN STREET, PENNINGTON, NJ 08534 USA SN 0013-4651 EI 1945-7111 J9 J ELECTROCHEM SOC JI J. Electrochem. Soc. PY 2015 VL 162 IS 3 BP A295 EP A299 DI 10.1149/2.0251503jes PG 5 WC Electrochemistry; Materials Science, Coatings & Films SC Electrochemistry; Materials Science GA CB7QZ UT WOS:000349823700008 ER PT J AU Vogl, US Lux, SF Crumlin, EJ Liu, Z Terborg, L Winter, M Kostecki, R AF Vogl, Ulrike S. Lux, Simon F. Crumlin, Ethan J. Liu, Zhi Terborg, Lydia Winter, Martin Kostecki, Robert TI The Mechanism of SEI Formation on a Single Crystal Si(100) Electrode SO JOURNAL OF THE ELECTROCHEMICAL SOCIETY LA English DT Article ID LITHIUM-ION BATTERIES; ORGANIC CARBONATE ELECTROLYTES; GRAPHITE NEGATIVE-ELECTRODES; NANO-SILICON ELECTRODE; THIN-FILM ELECTRODE; PLANE SURFACE-AREA; SOLID-ELECTROLYTE; FLUOROETHYLENE CARBONATE; PHOTOELECTRON-SPECTROSCOPY; NANOSILICON ELECTRODES AB A fundamental study of interfacial phenomena on a Si(100) single crystal electrode in organic carbonate-based electrolytes was carried out. The SEI formation on the Si(100) single crystal electrode was investigated as a function of the electrolyte composition, electrode potential and LixSi lithiation degree. Fourier transform infrared spectroscopy (FTIR) and X-ray photon spectroscopy (XPS) studies of the SEI layer during early stages of SEI formation indicate a strong dependence of the SEI composition on the electrolyte compo