September 2013 - Allocations-admins - mailman3.cels.anl.gov

[LCRC Accounts] Yearly Allocation Request from Hydro-model
by accounts＠lcrc.anl.gov 04 Sep '13

04 Sep '13

Hello, A yearly allocation for the LCRC cluster has been requested with the following updated information: Submitter/PI: Eugene Yan Project Name: Hydro-model Division: EVS Project title: Hydrologic modeling Associated funding: NASA; DOE EDER Other Systems: MCS UNIX machines Science: (1) Improve assessment of water resources and their response to climate change: case study for Africa continent; (2) Develop tool to improve hydrologic model calibration Project description: (1) Improve land surface model with GRACE data. Several experiment runs will be conducted to adjust parameters and reduce uncertainty with GRACE data. (2) Continue testing parallel calibration with SCE method and improve the efficiency of tool and ease of implementation. Project URL: Current FY Hours Used: undetermined amount New FY Requested allocation: 400000 Q1: 100000 Q2: 100000 Q3: 100000 Q4: 100000 Justification: Thank You, The LCRC Accounts System

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[LCRC Accounts] Project Request: dual-fuel-sprays
by accounts＠lcrc.anl.gov 03 Sep '13

03 Sep '13

Hello, A new project on the LCRC cluster has been requested. Please forward the information on to the LCRC Allocation sub-committee. Applicant's name: Zihan Wang Applicant's institution: ANL Applicant's division: Energy Systems Project Name: dual-fuel-sprays Project title: High-fidelity modeling of gasoline and diesel sprays in a Chrysler dual-fuel engine Associated funding: DOE - Office of Vehicle Technologies Other Systems: Chrysler Group LLC, Convergent Science Inc. Science: We have previously shown that Diesel Micro Pilot (DMP) combustion mode in a gasoline/ Diesel dual-fuel engine is promising to achieve both lower soot and NOx emissions over a wide range of engine load and speed. Under DMP conditions, gasoline is directly injected in the cylinder. Its spray pattern is critical to gasoline/ air mixing before ignition. The diesel fuel is the igniting source for the gasoline/ air mixture. Hence it is critical to understand both gasoline and diesel injection and mixture formation characteristics. This involves predicting the spray penetration and radial distribution accurately. Such information is available from x-ray radiography experiments performed at Argonne Advanced Photon Source. This x-ray dataset will be used to develop good correlations for gasoline and Diesel spray modeling set-up. With the use of parallel processing and highly-scalable CFD solvers, Large Eddy Simulation (LES), which directly resolves the large scales in the flow field, is able to provide more detailed local flow structures and “cycle-to-cycle” variations in both gasoline and diesel spray events. Project description: The project is divided into three major tasks to be performed in 12 months in collaboration with Chrysler Group LLC and Convergent Science Inc.: Task 1: Traditional Reynolds-Averaged Navier-Stokes (RANS) method will be applied to study non-evaporating gasoline and diesel sprays. Previously studied grid-convergence criteria will be implemented. Simulation results such as spray penetration, projected spray density, and Transverse Integrated Mass (TIM) will be validated against experimental measurements. Task 2: Large Eddy Simulation (LES) method with a couple of available sub-grid models will be applied to study spray events under the same conditions as Task 1. Previously studied grid-convergence criteria specific to LES will be implemented. Results will be compared to both RANS results and experimental measurements. Task 3: Sensitivity analysis on important spray parameters and ambient conditions and injection pressures will be investigated. Influence of spray model constants will be studied. The specific methods used for the multi-phase, reacting flow simulations with moving boundaries will include: 1) Finite volume schemes 2) LES (dynamic structure) and RANS turbulence models used 3) Detailed chemical kinetic models for diesel fuels 4) CONVERGE software is being used - ~120 licenses available 5) Scales well up-to 64 processors 6) Detailed spray models used for different spray processes Project URL: Requested allocation: 499000 Q1: 125000 Q2: 125000 Q3: 125000 Q4: 124000 Justification: The requester has used undetermined amount hours of their initial startup project. In addition to approving an initial amount, please specify a Category and Subcategory for this project. For a list of the current selection of approved categories, please see: https://wiki.lcrc.anl.gov/wiki/Processes/Categories Once the Allocation committee has approved the project, please go to the Project Management page to create it: https://accounts.lcrc.anl.gov/projects.php Thank You, The LCRC Accounts System

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[LCRC Accounts] Yearly Allocation Request from MBM
by accounts＠lcrc.anl.gov 03 Sep '13

03 Sep '13

Hello, A yearly allocation for the LCRC cluster has been requested with the following updated information: Submitter/PI: hakim iddir Project Name: MBM Division: MSD Project title: Modeling Battery Materials (MBM) Associated funding: EFRC, EERE Other Systems: EMSL-PNNL, CNM-ANL Science: Rechargeable Li-ion batteries (LIB) have become one of the most important energy storage devices for portable electronics, electric and plug-in hybrid vehicles, owing to their high energy density and design flexibility 1. Graphitic based materials are usually used for the anode in commercial LIB because of their low cost, relatively high capacity, non-toxicity, and improved thermal stability and safety over lithium metal anodes2, as a result of a passivation film (solid-electrolyte interface (SEI)) that forms on graphite3. Previous studies suggested that defects in disordered/amorphous graphene sheets might be at the origin of their greatly enhanced storage capacity2d, 4. A fundamental understanding of both SEI formation, structure and properties, as well as Li and Li+ diffusion across different defects in graphene planes is a prerequisite to better understand the overall capacity and transport behavior of several graphitic anode materials and configurations in LIB, such as carbon nanospheres 5, carbon nanotubes (CNT)6, highly oriented pyrolitic graphite and graphene paper7. This work will be closely coupled with extensive experimental efforts conducted by two groups from the Chemical Sciences and Engineering (CSE) division, as well as research groups from Northwestern University (NU) and the University of Illinois at Urbana-Champaign (UIUC). This project is being done as part of the ANL EFRC on energy storage and an EERE funded program. The new added component to this project involves the high capacity and energy-density electrodes that are needed to extend the range of lithium-ion-battery-powered PHEVs and EVs. A key feature of the layered-layered materials, nominally of composition xLi2MnO3•(1-x)LiMO2, is the structural compatibility of the monoclinic (Li2MnO3) and rhombohedral (LiMO2, M=Mn,Ni,Co, etc.) crystal structures, which both feature (strained) cubic-close-packed oxygen sublattices with comparable lattice constants. This compatibility enables synthesis of the composite material with coherent interfaces or even solid solution-like ordering, with domains that exhibit the atomic ordering characteristic of Li2MnO3 on nanoscale dimensions 8. The homogeneity of these highly integrated composites has posed obstacles to their characterization on an atomic scale. Although extensive modeling exists of the individual phases for the monoclinic phase, and for the rhombohedral phase, little simulation has b een performed for the composites. 1. Tarascon, J. M.; Armand, M., Issues and challenges facing rechargeable lithium batteries. Nature 2001, 414 (6861), 359-367. 2. (a) Noel, M.; Santhanam, R., Electrochemistry of graphite intercalation compounds. Journal of Power Sources 1998, 72 (1), 53-65; (b) Fauteux, D.; Koksbang, R., Rechargeable lithium battery anodes: alternatives to metallic lithium. Journal of Applied Electrochemistry 1993, 23 (1), 1-10; (c) Yazami, R.; Touzain, P., A reversible graphite-lithium negative electrode for electrochemical generators. Journal of Power Sources 1983, 9 (3), 365-371; (d) Yoo, E.; Kim, J.; Hosono, E.; Zhou, H.-s.; Kudo, T.; Honma, I., Large Reversible Li Storage of Graphene Nanosheet Families for Use in Rechargeable Lithium Ion Batteries. Nano Letters 2008, 8 (8), 2277-2282. 3. Aurbach, D., Electrode-solution interactions in Li-ion batteries: a short summary and new insights. Journal of Power Sources 2003, 119-121, 497-503. 4. (a) Pan, D.; Wang, S.; Zhao, B.; Wu, M.; Zhang, H.; Wang, Y.; Jiao, Z., Li Storage Properties of Disordered Graphene Nanosheets. Chemistry of Materials 2009, 21 (14), 3136-3142; (b) Sato, K.; Noguchi, M.; Demachi, A.; Oki, N.; Endo, M., A Mechanism of Lithium Storage in Disordered Carbons. Science 1994, 264 (5158), 556-558. 5. Pol, S. V.; Pol, V. G.; Sherman, D.; Gedanken, A., A solvent free process for the generation of strong, conducting carbon spheres by the thermal degradation of waste polyethylene terephthalate. Green Chemistry 2009, 11 (4), 448-451. 6. Frackowiak, E.; Béguin, F., Electrochemical storage of energy in carbon nanotubes and nanostructured carbons. Carbon 2002, 40 (10), 1775-1787. 7. Abouimrane, A.; Compton, O. C.; Amine, K.; Nguyen, S. T., Non-Annealed Graphene Paper as a Binder-Free Anode for Lithium-Ion Batteries. The Journal of Physical Chemistry C 114 (29), 12800-12804. 8. Croy, J. R.; Gallagher, K. G.; Balasubramanian, M.; Chen, Z.; Ren, Y.; Kim, D.; Kang, S.-H.; Dees, D. W.; Thackeray, M. M., Examining Hysteresis in Composite xLi2MnO3•(1–x)LiMO2 Cathode Structures. The Journal of Physical Chemistry C 2013, 117 (13), 6525-6536. Project description: As indicated in our LCRC Fusion annual report (2013) for the MBM project, extensive Density Functional Theory (DFT) and Ab-Initio Molecular Dynamics (AIMD) calculations on both metallic and semiconducting SWCNTs have been performed. We investigated the binding of CO, OH to Pt(100) strained oxide nanofacets. We initiated studies of Mn and Mn2+ diffusion through di-vacancies (DV) in graphene as well as in crystalline Li2CO3 to determine the migration path and the overall potential energy profile. Li and Li+ diffusion through defects sites in graphene, work already in progress, which requires further investigation in relation to system size, and comparison to Mn/Mn2+ diffusion studies. We have also started a new project within the MBM on layered-layered composites cathode materials, where the end goal is to understand and perhaps design new materials that would suppress the voltage fade problem encountered with the utilization of the current composites in Li-ion batteries. In this project we will investigate the stability of several hexavalent dopant candidates and their migration in both Li2MnO3 and LiMO2 phases of the composite, in the presence of Li and O vacancies. The preliminary diffusion studies of Co and Mn show that the Nudged Elastic Band (NEB) method does not always capture the physics behind the migration, such as the disproportionation observed with Co vacancy migration. Constrained migration calculations will be necessary to capture the disproportionation effect during the migration of the transition metal. A total of about 600000 core hours would be needed to complete this project. Project URL: Current FY Hours Used: undetermined amount New FY Requested allocation: 600000 Q1: 150000 Q2: 150000 Q3: 150000 Q4: 150000 Justification: Mn and Mn2+ diffusion in Li2CO3 and DV in graphene will require about 200000 hours. We will use both the NEB and the constrained methods to determine the migration barriers. Several calculations will be required to investigate the effect of charge and spin during the migration. Supercells with 192 atoms (1 Li layer, 1 TM layer and 2 O layers) will be used for the doping studies, and migration studies of M and Li within the layers of Li2MnO3-LiMO2 composites. Larger supercells (doubled in the c direction, i.e. double the number of layers in the cell) with 384 atoms will be required for the migration studies between the layers, that will involve more (Li, O) vacancy configurations and the Li-M dumbbell configuration. As mentioned above, both NEB and the constrained techniques will be used in this study. NEB calculations are lengthy and expensive; particularly when DFT+U spin polarized calculations are needed. 400000 hours will be ne necessary to run these calculations. Thank You, The LCRC Accounts System

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[LCRC Accounts] Yearly Allocation Request from ECG_LiAir
by accounts＠lcrc.anl.gov 03 Sep '13

03 Sep '13

Hello, A yearly allocation for the LCRC cluster has been requested with the following updated information: Submitter/PI: Mike Welland Project Name: ECG_LiAir Division: MSD Project title: Mesoscale modeling of electrochemical crystal growth for Li-air batteries Associated funding: Atomistically Informed Mesoscale Modeling for Advanced Electrical Energy Storage Systems Other Systems: Science: This work involves mesoscale simulations of oxide growth in Li-air batteries by modeling multicomponent mass transport, electrostatics, structural mechanics, and microstructure evolution. We are developing a new continuum scale model that considers large variations in constituent concentrations between phases, concurrent diffusion on substitution and interstitial lattices, and an original phase-field formulation. The study encompasses electrochemical crystal growth / dissolution as well as nanoscopic interfacial effects such as the electric double layer. In application to realistic systems, we seek to understand the factors influencing the performance, longevity and behavior of Li-air and similar advanced battery concepts. Project description: The model is derived from a thermodynamic description of the system as a functional of the concentration of ionic species (Li+, O2-, A- and e-) and a neutral solvent, the electrostatic potential, the local phase, and the local pressure. Working through the theory of irreversible processes, we can describe the electrochemical growth / dissolution process in a system of at least eight highly non-linear, coupled partial differential equations which must be solved numerically via the finite element method. We have selected the FEniCS package for this purpose, which is an open-source project developed by teams internationally and relies on the PETSc library for calculation, thus taking advantage of the latters scalability and efficiency on computer clusters. We have developed a phase-field formulation with a newly developed technique of calculating extreme concentration variations, on the order of 1023 over a simulated interface width of 1Å, in a numerically robust fashion [1]. The model is currently implemented in 1D in order to have fast turnaround in simulation results while the theory and implementation were being developed. Figure 1 shows a simulations of the ideally polarized electrode which naturally produces the electric interfacial double layer, a distinctly mesoscopic phenomenon and an important interfacial phenomenon for electrical energy storage systems. The 1D implementation is useful for exploring the physics of the problem and developing the model, however in real systems, the interface morphology is complex and requires 2- or 3-D simulations. Due to the high resolution required by the phase-field model to accurately represent the phase boundary, problems of this sort are computationally expensive. It is this feature, and the non-linear nature of the problem, which motivates running this code on high performance computers in order to obtain results of sufficient size to be practically important within a reasonable timeframe. To the author’s knowledge, multidimensional microstructural studies of such systems have not been done to this level and would constitute a novel application to a popular and important field of scientific research. Project URL: http://cmcsn.phys.washington.edu/content/computational-microstructure-scien… Current FY Hours Used: undetermined amount New FY Requested allocation: 400000 Q1: 50000 Q2: 100000 Q3: 100000 Q4: 150000 Justification: Thank You, The LCRC Accounts System

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[LCRC Accounts] Yearly Allocation Request from dynamics
by accounts＠lcrc.anl.gov 03 Sep '13

03 Sep '13

Hello, A yearly allocation for the LCRC cluster has been requested with the following updated information: Submitter/PI: Gary Leaf Project Name: dynamics Division: MCS Project title: Dynamics of biophysical systems. Associated funding: DOE Other Systems: MCS workstations, Beagle at Computation Institute Science: We investigate reduced models for the selective adsorbtion of various competing cations in neuronal sodium channels. The selection of one type of cation over another is basic for successful biological function. Starting with a reduced model for a sodium channel, develop and implement algorithms for the selectivity filter which is that portion of the ionic pathway that determines the selectivity. At this time the numerical simulations are based on using Grand Canonical Monte Carlo combined with determining the energetics of ion transport in the channel filter. Selectivity is determined by the free energy as described by the excess chemical potential which is generated by various physical effects in the channel filter such as polarization, ion size, ion charge, dielectric screening, etc. Calculating the magnitude of these components provides insigjy into the selectivity mechanisms. Project description: The goal of our computations for the reduced model of a sodium channel is to compute the dependence of the free energy components for the channel. We investigate the dependence on such factors as channel size, cation size in relation to channel size, ion charge, protein polarization effects, and polarization effects in the channel. The object is to gain a deeper understanding of the selectivity mechanism whereby some ions are selected over others for transport through the channel. This is in spite of the difference in concentration outside the channel. Our computations are based on using a Grand Canonical Monte Carlo (GCMC) scheme to compute the free energy components as well as the expected ionic concentration in the filter portion of the channel. For a given state (configuration and parameter settings) we compute a multiple set of final realizations in parallel. The number of realizations ranges from 24 to 48 with 32 being the usual number. We expect each GCMC calculation will require on the order of 40K steps with 50-70 particle insertion/deletion attempts as part of the free energy calculation. Our computational study will divided into three main segments. Each segment has three parts that are essentially the same for each segment. Segment I. Here we model with a homogeneous dielectric; so that there is no polarization effects from either the protein or the or the channel. The object is to isolate the effect of excluded volume on selectivity. Because this model is homogeneous, the computations are relatively short. On the order of 8 hours per calculation. Part A. Vary the filter pore radius: R = 3.0 3.5 4.0 4.5 5.0 Angs Part B. Vary the type of cation competing with sodium. Part C. Study the transmission of sodium over calcium for a sodium channel by gradually titrating calcium into the system. Because the this model homogeneous, the computations are very modest. We estimate that the study for segment I will require on the order of 4000 core-hours using 32 cores per computation. Cost: 4000 core-hours for Segment I study. Segment II. Study the role of protein polarization by varying the protein dielectric. This model is inhomogeneous, hence considerably more computationally expensive. This study has the same three parts as Segment I, but more calculations for each part as well as the increased cost of each run. We estimate that this portion of the study will involve about 60 cases covering the parameter ranges. Using 32 cores, although 48 may be needed, each will require on the order of 1664-2496 core-hours. Based on 60 cases this yields Cost : 99840-149760 core-hours for Segment II study Segment III. Study the role of polarization in the sodium channel by varying the channel dielectric. These cases also involve an inhomogeneous model; thus the cost will be comparable to the cost of the study in Segment II. Cost : 99840-149760 core-hours for Segment III study. Project URL: http://www.phys.rush.edu/RSEisenberg/physioeis.html Current FY Hours Used: undetermined amount New FY Requested allocation: 360000 Q1: 90000 Q2: 90000 Q3: 90000 Q4: 90000 Justification: Thank You, The LCRC Accounts System

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New LCRC report submitted for Drude
by support＠lcrc.anl.gov 03 Sep '13

03 Sep '13

Full project report at https://accounts.lcrc.anl.gov/reporting/project/2013/?project=Drude

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[LCRC Accounts] Yearly Allocation Request from Raney_Nickel
by accounts＠lcrc.anl.gov 03 Sep '13

03 Sep '13

Hello, A yearly allocation for the LCRC cluster has been requested with the following updated information: Submitter/PI: John J. Low Project Name: Raney_Nickel Division: MCS Project title: A Molecular Model of Raney Ni Associated funding: None Other Systems: None Science: Raney nickel is a nanostructured catalyst which is used in a variety of industrial processes and organic syntheses such as hydrogenation reactions. The basis forms a NiAl alloy which is transformed into the active form by leaching out aluminum which leads to the characteristic porous structure of the final catalyst. The porosity depends on the initial composition of the NiAl alloy which is typically prepared by melting nickel together with aluminum and subsequent quenching. The quenching process induces the formation of different NiAl phases which react differently with the caustic and thus affect the pore formation in the final catalyst. Experimental studies indicate that the sponge-type structure of Raney Nickel grains is formed by a collection of crystallites adhering together. Since the structure of both the precursor alloy and the active form of Raney Nickel is determining the catalytic activity and performance, it is crucial to gain a detailed understanding of the structural properties at the atomistic level. The goal of this project is to leverage molecular modeling to provide critical insights into how the composition of the precursor alloy affects the porosity and thus activity of Raney Nickel. Project description: During the first phase of the project, molecular dynamics (MD) simulations have been performed on fusion using the LAMMPS software package in order to analyze the influence of the initial composition of the alloy on the structural properties of the precursor. Model structures for four different compositions (40/50/60/70 wt% Ni) have been created using Scienomics MAPS platform by randomly replacing Ni and Al in the corresponding fractions in a NiAl3 supercell. In order to ensure a statistically relevant sampling, five initial starting configurations have been generated for each of these model structures. The structures were equilibrated at 2000 K and then cooled down to room temperature over 1 ns as described by Noya, et al. [J. Non-Crystal. Solids 298, 60–66 (2002)]. The MD simulations performed so far provided insight to what extent the initial configuration and compositions affects the structure of the precursor. The analysis density and cell parameters of the final structures indicates that the composition has a significant influence, while the configuration has only a very minor impact. In general, the density, cell parameters, total energy and volume over the simulation time show a consistent behavior. The final structures as obtained from the quenching simulations will serve as basis for additional MD simulations and equilibrated for 1 ns at room temperature to ensure convergence. The trajectories will be analyzed with respect to the formation of nanostructured clusters based on a next neighbour search, for which MAPS scripting facilities will be used. The trajectories will be analyzed with respect to the formation of nanostructured clusters. In addition we plan to ues the open source program RINGS (http://rings-code.sourceforge.net] will be used to analyze local structural environments and voids. From each model, Al will be removed and only 5-10 % Al will be left which corresponds to the experimentally observed final catalyst composition. These porous models will be minimized, which will only require a few hundred core-hours, and afterwards analyzed with regard to pore size, pore distribution, and accessibility from surface for the various compositions and initial config urations to explore trends that can be linked to the catalytic performance. In this way, we can gain a fundamental understanding about the formation of nanostructures in the precursor alloy in dependence of the initial composition. In the laboratory, the precursor is activated though treatment with sodium hydroxide leaching out the majority of the Al and leading to structural re-arrangements of the Ni bulk. This process will not be simulated as it is beyond the scope of the present project. Instead, we will focus on modeling the structure of the final catalyst. To provide a reliable description of the nanoporous structure, large system sizes will be required which will also allow to capture effects of grain boundaries that a supposed to be important for the chemistry of the final catalyst. The computational time needed for performing MD simulations and analyzing the trajectories of all 20 models will be considerable. Each model structure contains more than 65,000 atoms. According to the LAMMPS Cu benchmarks[ http://lammps.sandia.gov/bench.html#eam] 100 steps for a system size of 32,000 atoms would take 0.3 s (fixed CPU time) on 512 cores. A 1 ns trajectory (1,000,000 steps) for 32,000 atoms would take 500 core-hours and a 65,000 atom system about 1250 core-hours. 25,000 core-hours will be needed for the simulations of the 20 alloy model structures. Characterization studies of Raney Nickel by Anderson’s group and others which yield a qualitative picture of Raney Nickel. [J. Cat. 16, 281–291 (1970)] The void volume of these particles ranges from 0.05 to 0.15 cc/g. X-ray diffraction and X-ray Absorption Spectra show that local structure of Raney Ni’s is similar to FCC Ni. Fouilloux gives a qualitative description of Raney Nickel as a spongy material composed of 100 nm agglomerates of smaller 2.5 to 15 nm nanocrystals. Our model of Raney Nickel starts with 500 randomly packed 12.5 Å spherical nanocrystallites of Nickel in a 100 nm sphere. The procedure of Lubachevsky, et al. will be used to generate random packing of the spheres.[J. Stat. Phys. 64 501–524 (1991)] Since random close packing has a density of approximately 0.63, this model will have a void volume (0.06 cc/g) similar to Raney Ni. The initial positions of the atoms in the Ni nanospheres will be created from a randomly oriented and shifted FCC latt ice. The final structure will be determined through simulated annealing and the EAM potentials as implemented in LAMMPS. Our model should be qualitatively similar to experimental structure of Raney Nickel. These structures will be tested by comparing calculated properties from the predicted structure to the experimentally determined pore size distribution, heterogeneities from small angle X-ray scattering and line broadening in X-ray diffraction. Several modeling studies of grain boundaries use molecular dynamics to generate structures. Van Swygenhoven and Caro used a stochastic procedure that starts with randomly placed seed particles with the rest of the space filled with a Voroni construction.[Phys. Rev. B 58, 11246–11251 (1998)] Keblinski randomly placed seed particles in a liquid metal and then quenched the melt to generate a model crystal with grain boundaries. [Scr. Mater. 41, 631–636 (1999)] These procedures yield a model of a solid composed of nanocrystalline grains. We will follow the spirit of these modeling approaches by randomly placing seeds of Ni crystallites in a gas (or liquid) of Ni atoms and use simulated annealing to generate a low energy structure. Raney Nickel, which has a void volume of 0.1 cc/g, is essentially half void by volume. A simple model would be to seed a gas with a density half that of Ni metal. The gas will condense on the seed crystallites and create an agglomerate with the appropriate void volume. Since the condensation is exothermic, a Nose or Andersen thermostat will keep the temperature below the melting temperature (1728K) of Ni during the simulation. Starting at 1500 K and scaling the temperature to 0K over 100 picoseconds will quench to a low energy structure through simulated annealing. Since the low energy structure will create particles which have the density of Ni metal, the voids between the particles should have half the volume of the initial volume. The number of crystallites should control the size of the nanocrystals formed during simulated annealing. A careful choice of initial conditions should lead to the desired size of nanocrystals and void volumes. The RINGS program will allow a systematic and analytical analysis of these structures. A 100 nm droplet of Ni with half the density of bulk Ni is a model of Fouilloux’s description of Raney Nickel.[J. Cat. 25, 212 (1972)] The scale of this calculation would be significant. The model would be initiated by randomly placing 500 seed crystallites (Ni55 clusters) in a hundred nanometer sphere and then randomly inserting 25 million atoms into the space between the seeds. The embedded atom method as implemented in LAMMPS can handle simulated annealing of models of this size. The Cu EAM benchmark on the LAMMPS website shows that 100 steps of molecular dynamics for 16 million atoms could be done on 512 cores of a Xeon/Myrinet cluster in 21 seconds. [http://lammps.sandia.gov/bench.html#eam] A 100 picosecond trajectory (100,000 steps) would take 60 hours (30,000 core-hours). Fusion or Blues have faster processors and an InfiniBand interconnect that will yield better performance. The estimated CPU requirements derived from timings for the Xeon/Myrinet cluster is an upper bound. We anticipate repeating this calculation a few times with three different compositions requiring 100,000 core-hours. Our initial calculations will use a periodic model containing a million atoms and 20 seeds to verify this approach will give morphology similar to Raney Nickel. The test will involve comparing calculated properties from the predicted structure to the experimentally determined pore size distribution, heterogeneities from small angle X-ray scattering and line broadening in X-ray diffraction. [J. Cat. 23, 286 (1971), Cat. Today 163, 13–19 (2011)] If this model does not yield a satisfactory result we will implement and test a stochastic Voroni procedure. [Phys. Rev. B 58, 11246–11251 (1998)] These calculations will require a few thousand core hours and will not exhaust our allocation before developing a working model. Once we have established a procedure that generates a model of a porous solid composed of nanocrystalline grains, we will carry out calculations on a more realistic 50 million atom droplet model of Raney Ni. 50,000 core hours will be needed for these experimen ts with smaller periodic models. We will use EAM to model hydrogen adsorption on our model of Raney Nickel. The model will have monolayer coverage (one hydrogen atom per surface Ni atom). The surface will be defined by Ni atoms with coordination less than twelve. Simulated annealing will be use to find a low energy distribution of hydrogen on the surface of Raney Ni. The predicted binding energies, vibrational frequencies and geometries will be used to classify the chemisorption sites to a smaller number of representative sites. 50,000 core-hours will be required for the chemisorption models. The pore size, pore distribution, and the accessibility of the droplet model and chemisorbed model will be compared with the results obtained for the precursor models. This strategy will allow to explore to what extent the nanostructural agglomerations in the precursor are reflected in the porous active form. The generalized chemisorption sites will form the basis of smaller periodic models. We will use the smaller models to model hydrogenation of benzene on Raney Nickel with an electronic structure program like abinit, bigdft, cp2k or qbox. These calculations will be done in a future project. Overall, 200,000 core-hours will be needed over a period of five months for performing the in silico experiments for the project. About Scienomics Scienomics was established in 2004 and with selected partnerships with the best-of-the-breed (e.g.: Sandia National Labs, Max Planck Institute, Fraunhofer Institute, University of Illinois, Demokritos, University of Shanghai), Scienomics’s MAPS platform offers a unique and powerful blend of multiscale and multiparadigm modeling and simulation modules. With high quality science and industrial solution oriented applied research, Scienomics has garnered collaborative projects with companies in the areas of energy and green chemistry, alternate fuels, catalysis, polymers, biodefense, auto exhaust, etc. Biography of Relevant Members John J. Low, Principal Computational Science Specialist at Argonne National Laboratory has a Ph.D. in Chemistry from the California Institute of Technology. After graduation John worked at UOP LLC, a Honeywell Company. His work at UOP focused on modeling and characterization of catalysts and adsorbents used in the petrochemical industry, hydrogen storage and carbon sequestration. John supports the computational chemistry applications at high performance computers and performing research on Li-Ion batteries, converting biomass to fuels, and nuclear materials at Argonne. He is expert in quantum chemistry, molecular dynamics and Monte Carlo methods on high performance computers. Dr. Sabine Schweizer, Senior Scientist at Scienomics has a Ph. D. in Theoretical Chemistry from University of Tuebingen, Germany. Her work experience is in the area of applying quantum chemical methods to large and small molecules. Her experience is particularly useful in the areas of homogenous and heterogenous catalysis, where energetics and dynamics play an important role in the reactions. She has experience working with multiscale hybrid methods combining quantum chemical and classical methods which makes her particularly versatile in applying Scienomics’ multiscale, multiparadigm MAPS platform to study hard materials such as surfaces, coatings, semiconductors, solar cells, etc. Dr. Lalitha Subramanian, Chief Scientific Officer and VP of Services has 18 years of experience providing insight into chemical systems and processes that are of critical interest to industry. Following her Ph. D. in Chemistry, her post-doctoral work was with Prof. Roald Hoffmann (Nobel Laureate) at Cornell University. She has been a leading architect of solutions in the areas of alternate energy, catalysis, materials design, and process optimization. She has worked on numerous proprietary projects for diverse companies and in this pursuit; she has delivered product enhancements, process optimization and cost savings to her customers. Lalitha maintains a broad range of partnerships in oil & gas, chemical, personal care, materials, semiconductors, automotive, aerospace, and pharmaceutical industries. She has co-authored a book on software techniques used in Materials Science published by CRC Press, 2005. She continues to present invited lectures and has numerous scientifi c publications. Recent References: Kimberly-Clark Corporation use Scienomics software and services for predicting properties of new polymer systems (2012). US Army Research Lab use Scienomics software and services for proprietary research on polymeric systems (2012). Materials Engineering Research group at Purdue University used Scienomics software suite for studying the crosslinking process of thermosetting polymers (2010). Project URL: Current FY Hours Used: undetermined amount New FY Requested allocation: 200000 Q1: 50000 Q2: 50000 Q3: 50000 Q4: 50000 Justification: Thank You, The LCRC Accounts System

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[LCRC Accounts] Yearly Allocation Request from Redoxshuttles
by accounts＠lcrc.anl.gov 03 Sep '13

03 Sep '13

Hello, A yearly allocation for the LCRC cluster has been requested with the following updated information: Submitter/PI: Paul Redfern Project Name: Redoxshuttles Division: CSE Project title: Redox Shuttles and Additives for Lithium-Ion Batteries Associated funding: EERE-DOE Other Systems: Small Group Cluster Science: There are several types of electrolytes that are used to improve the performance of the batteries. Some electrolyte additives are used to improve lithium-ion battery performance by facilitating solid-electrolyte (SEI) formation, reducing irreversible capacity and gas formation, improving thermal stability, protecting cathode materials, improving electrolyte properties, decreasing flammability and providing overcharge protection. It is also desirable to develop additives that can stabilize electrolytes near 5 V in order to deliver energy at higher density and potential. Numerous additives have been developed that improve some aspect of battery performance, but many introduce negative side effects. A second type is used to prevent dangerous overcharge of lithium-ion batteries occurs when charge from current forced through a cell exceeds its charge storing capability, leading to chemical and electrochemical reactions, rapid temperature rise, self accelerating reactions and explosion. Redox shuttle molecules are additives that are reversibly oxidized and reduced at potentials slightly higher than the end of charge cathode potential, locking the cathode potential at the oxidation potential of the redox shuttle and thereby preventing overcharging. The shuttling mechanism can be regarded as an internal short that can be repeated continuously due to reversible oxidation and reduction of the shuttle molecule. Redox shuttles with excellent performance and compatibility are critically important to the development of lithium-ion battery technology. Development of new redox shuttles is difficult and has been largely based on trial and error due to the multidisciplinary knowledge r equired. Ideal redox shuttles should be electrochemically reversible, have a redox potential slightly higher than the cathode end of charge potential, be electrochemically stable, have good solubility and high diffusion coefficients, and be compatible with the cell, i.e., they should not adversely affect normal cell performance. The shuttle should not react with electrolytes, the solid-electrolyte interface, separators, current collectors, binders, etc. Interface resistance and thermal properties should also be considered. Project description: Over the past year we have examined many redox shuttles and electrolytes for high voltage applications. Calculations were performed on several substituted quaterphenyls. Oxidation potentials were found to be sensitive to the position of substituent and the effects are approximately additive even when substituents have opposite push-pull effects. Hammett sigma parameters were also calculated. In collaboration with experimentalists we developed a new platform to build redox shuttles involving a fused cyclohexene ring on a benzene ring. Numerous high voltage electrolyte candidates were also examined including lactones, cyclic sulfates and fluorinated species. Electrolytes with high dielectric constants and electron withdrawing groups such as F or SO2 have increased oxidative stability. There are still many avenues to be explored. Quantum chemical calculations will be used to calculate additive oxidation and reduction potentials and to investigate mechanisms of solid-electrolyte interface formation and additive decomposition reactions. Effects of electron donating and withdrawing groups on additive performance will be investigated. Oxidation potentials and decomposition reactions of redox shuttles will be determined. Benchmark calculations using high level ab initio approaches such as G4 will be performed. Oxidation and reduction potentials are calculated by optimizing the geometries of the neutral and ionic species with B3LYP/6-31G*, followed by frequency calculations to get the gas phase free energies. Then solvation effects are taken into account using a single point B3LYP/6-31+G* pcm calculation with the default (water) solvent and a dielectric constant of 55.725 representing the electrolyte (25% EC, 25% ethyl methyl carbonate, 50% PC). Finally basis set effects are taken into account with a B3LYP/6-311+g(3df,2p) single point calculation. From these results the total free energy of each species is calculated as electronic energy plus gas phase free energy plus solvation free energy. The free energies of the neutral and ionic species are then subtracted to get an absolute free energy difference. During this process the electron affinity (reduction potential) or ionization potential (o xidation potential) is calculated. We intend to evaluate at least 200 redox shuttles including biphenyls and terphenyls and fused hexene ring substituted benzenes. High redox shuttle oxidation potentials are required for high voltage applications. We will also examine at least 200 SEI additives including carbonates, anhydrides, imides, cyclic phosphates, and borates, as well as many others. Reduction potentials of SEI additives must be higher than the electrolytes. Using theoretical results, databases will be developed to screen for new additives using quantitative structure-property relationships and physical organic chemistry principles. New redox shuttles and SEI additives will be developed for high voltage applications. Software We intend to use Gaussian 09 for quantum chemical calculations. In Gaussian 09 the DFT calculations scale well up to 64 processors, however the high-level ab initio methods scale only up to 16 processors. Therefore these calculations do require a longer execution time. Publications 1) Asymmetric form of redox shuttle based on 1,4-di-t-butyl-2,5-dimethoxybenzene, Wei Weng, Yunting Tao, Zhengcheng Zhang, Paul C. Redfern, Larry A. Curtiss, and Khalil Amine, accepted. 2) Fluorinated electrolytes for 5 V lithium-ion battery chemistry, Zhengcheng Zhang, Libo Hu, Huiming Wu, Wei Weng, Meiten Koh, Paul C. Redfern, Larry A. Curtiss and Khalil Amine, Energy Environ. Sci., 2013, 6, 1806. 3) Smart Polymeric Cathode Material with Intrinsic Overcharge Protection Based on a 2,5-Di- tert butyl-1,4-dimethoxybenzene Core Structure, Wei Weng , Zhengcheng Zhang , * Ali Abouimrane , Paul C. Redfern , Larry A. Curtiss , and Khalil Amine, Adv. Funct. Mater. 2012, DOI: 10.1002/adfm.201200458 4) Molecular engineering towards safer lithium-ion batteries: a highly stable and compatible redox shuttle for overcharge protection, Lu Zhang , Zhengcheng Zhang , Paul C. Redfern , Larry A. Curtiss and Khalil Amine, Energy Environ. Sci., 2012, 5, 8204-8207. 5) Improved synthesis of a highly fluorinated boronic ester as dual functional additive for lithium-ion batteries, Wei Weng; Zhengcheng Zhang; Schlueter, J.A.; Redfern, P.C.; Curtiss, L.A.; Amine, K., Journal of Power Sources, 2011, 196, 2171-2178. 6) Fused ring and linking groups effect on overcharge protection for lithium-ion batteries, Wang, W (Wang, Wei)1; Zhang, ZC (Zhang, Zhengcheng)1; Redfern, PC (Redfern, Paul C.)1; Curtiss, LA (Curtiss, Larry A.)1,2,3; Amine, K (Amine, Khalil)1, JOURNAL OF POWER SOURCES, 2011, 196, 1530-1536. 7) Understanding the redox shuttle stability of 3,5-di-tert-butyl-1,2-dimethoxybenzene for overcharge protection of lithium-ion batteries, Zhengcheng Zhang; Lu Zhang; Schlueter, J.A.; Redfern, P.C.; Curtiss, L.; Amine, K., Journal of Power Sources, 2010, 195, 4957-4962. Project URL: Current FY Hours Used: undetermined amount New FY Requested allocation: 400000 Q1: 100000 Q2: 100000 Q3: 100000 Q4: 100000 Justification: Thank You, The LCRC Accounts System

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[LCRC Accounts] Yearly Allocation Request from qmc_for_nuclei
by accounts＠lcrc.anl.gov 03 Sep '13

03 Sep '13

Hello, A yearly allocation for the LCRC cluster has been requested with the following updated information: Submitter/PI: Robert Wiringa Project Name: qmc_for_nuclei Division: PHY Project title: Quantum Monte Carlo Calculations of Light Nuclei Associated funding: DOE Office of Nuclear Physics Other Systems: ANL Blue Gene/P (INCITE 30M hours for 12C studies) Science: This project uses Quantum Monte Carlo [Green's function (GFMC), variational (VMC), and auxiliary-field diffusion (AFDMC)] methods to compute ground-state and low-lying excited-state expectation values of energies, densities, electroweak transitions, spectroscopic overlaps, astrophysical reaction rates, etc., for light nuclei and low-energy scattering reactions involving these nuclei. Realistic two- and three-nucleon potentials are used. Our goal is a description of all of these systems using a Hamiltonian that also provides an excellent description of nucleon-nucleon scattering and nucleonic matter. Such a `standard nuclear model' can then be used, for example, to compute low-energy astrophysical reactions which cannot be experimentally measured. We are also actively engaged in making predictions that can and are being tested at experimental facilities such as ATLAS, NSCL, TRIUMF, and JLab. Project description: A) Electroweak moments and transitions We are studying a variety of electroweak properties and transitions in light p-shell nuclei, including both one- and two-body charge and current operators that include the effect of meson-exchange currents. We are nearing completion of work on electromagnetic transitions in 8Be and have started calculations for moments and M1 and M3 transitions in A=10 nuclei. We are also studying transitions in A=8 nuclei in co-operation with experimentalists in Mumbai and in A=10 with an experimental group at ATLAS, and finding they may provide new constraints on three-nucleon forces. We have started work on longitudinal and transverse response functions, which have not previously been studied for A>7 nuclei. We expect to use 120,000 core hours for this work in FY14. B) A=11,12 nuclei Extensive effort has gone into GFMC calculations of 0+ states in 12C using Intrepid and Mira, but only a few exploratory calculations of other A>10 nuclei have been made. We have some simple initial trial functions for 11Li and 11B, but other cases like 11Be and 12Be remain to be studied, particularly wave functions that are "clusterized." The VMC codes for these trial functions are running more efficiently from using a mix of OpenMP inside nodes (and benefitting from the larger memory within a Blues node) and MPI between nodes. We are also continuing studies of unnatural parity and intruder states in A=10 nuclei. We would like 120,000 cpu hours for this work in FY14. C) Asymptotic normalization coefficients and resonance widths for alpha-decay In the last few years we have developed a new method for evaluating asymptotic normalization coefficients (ANCs) that characterize the long-range tails of nuclear bound states and are the key determinant in low-energy astrophysics reaction rates. The calculation uses a short-range integral technique that can make do with relatively simple variational wave functions. A variant of this method allows the calculation of widths of narrow unbound states. The method has been applied to single-nucleon emission up to A=9 nuclei. We are adapting the method for alpha-particle emission and plan to study ANCs and widths nuclei up to A=10. We will need 40,000 hours for this work in FY14. D) Nucleon momentum distributions in A<=12 nuclei We have developed algorithms for evaluating one- and two-nucleon momentum distributions in nuclei using variational wave functions. These have often been requested by groups at JLab, both for analyzing past experiments and planning new ones. We wish to extend these calculations to the two-nucleon momentum distributions in 12C, which are relevant to recent two-nucleon knockout experiments, and to try incorporating the more exact GFMC wave functions. We would like 40,000 core hours for this work in FY14. E) Euclidean response of nuclei We are adding the ability to compute electromagnetic and neutral-current Euclidean response to the GFMC code. The code development is being done on Blues and production calculations for 4He will also be done there. Production for 12C will be done on Mira. The latter is of great interest for neutrio scattering in detectors and supernovae. This work should need 10,000 hours and will mostly be done in the first two quarters. Project URL: http://www.phy.anl.gov/theory/research/forces.html Current FY Hours Used: undetermined amount New FY Requested allocation: 330000 Q1: 85000 Q2: 85000 Q3: 80000 Q4: 80000 Justification: Thank You, The LCRC Accounts System

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[LCRC Accounts] Yearly Allocation Request from UNEDF_Optimization
by accounts＠lcrc.anl.gov 03 Sep '13

03 Sep '13

Hello, A yearly allocation for the LCRC cluster has been requested with the following updated information: Submitter/PI: Jason Sarich Project Name: UNEDF_Optimization Division: MCS Project title: Optimization for the NUCLEI SciDAC-3 Associated funding: DOE ASCR/NP/NNSA SciDAC-3 project NUCLEI DOE ASCR SciDAC Institutes FASTMath and SUPER Other Systems: Science: The NUCLEI (NUclear Computational Low-Energy Initiative) project will build upon recent successes in large-scale computations of atomic nuclei to provide results critical to nuclear science and nuclear astrophysics, and to nuclear applications in energy and national security. The large-scale computations we envision will transform the fields of low-energy nuclear physics and astrophysics. Physics topics to be addressed include nuclear interactions and their uncertainties, ab-initio studies of light nuclei and their reactions and of nucleonic matter and its astrophysical properties. We will also fundamentally advance the studies of neutron-rich nuclei and the fission of heavy nuclei, and the key nuclear physics issues in neutron stars and tests of fundamental symmetries. Project description: We are building upon our optimization successes under the SciDAC-2 UNEDF (Universal Nuclear Energy Density Functional) project in the successor project NUCLEI. In this project, optimizations over parameter spaces corresponding to energy density functional parameters will be performed using the Argonne-developed POUNDERS optimization algorithm. We will work with DFT codes HFBTHO and HFODD and begin work with ab initio codes such as MFDn. These physics codes will be run using parallel resources, in some cases with each of 100 nuclei being run on a separate node, in others (such as with MFDn), a simulating a single nucleus will require up to hundreds of nodes. In the past we have used OpenMP at the nucleus level in concert with library and compiler-based optimizations to bring the wall-clock time of a single by a factor 10. We will continue such code optimizations for the next-generation codes developed under NUCLEI. We anticipate using 40k core-hours for this task in FY14. For our parameter optimizations, we typically have 10-20 parameters and require on the order of 300 simulations. Based on the current simulation time, we would thus require 120 8-core nodes for up to 6 hours, or 6k core-hours for each version of the functional we want to optimize. We expect the number of core-hours will remain the same when using the new 16-core nodes. Past experience has let us to expect to do roughly 40 such optimizations in FY13, for a total of 240k core-hours for this task. POUNDERS is available in the Toolkit of Advanced Optimization (TAO), but we still prototype specialized versions of the algorithm using MATLAB/Octave on a single, master node. We will test updates to the TAO version on Blues and compare the performance and correctness against the MATLAB/Octave versions. As in the past, we will have roughly 4 users for this project. Project URL: http://computingnuclei.org Current FY Hours Used: undetermined amount New FY Requested allocation: 280000 Q1: 70000 Q2: 70000 Q3: 70000 Q4: 70000 Justification: N/a Thank You, The LCRC Accounts System

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