Simulations of Complex Chemistry at Mineral/Fluid Interfaces: Development and application of Petascale/Exaflop First Principle Simulation Technology
EMSL Project ID
49691
Abstract
Novel first principle methods of simulations will be developed and applied to computationally intractable geochemical problems such as: i) Interpretations of structure, reactivity and electron transport in mineral/fluid interfaces for complex highly correlated transition metal oxide minerals. This will include new computational tools for the analysis of nuclear magnetic resonance imaging (NMR) and synchrotron X-ray scattering observations (CTR) of the surface interface regions; ii) Develop simulation methods for the interpretation of NMR, EXAFS, XANES, and XRD spectra of aqueous solutions species thereby supporting the development of robust thermodynamic models of reservoir fluids. The collection and analysis of new data for important systems (Al3+(aq) and Mg2+(aq)) that have just become possible to observe with EXAFS and XANES is included in this program; iii) Develop free energy methods to efficiently sample fluid and interface structure. This software will support the prediction of the mechanisms of electron transfer, the structure of nano-materials and identify reaction mechanisms in the difficult to probe interface region; and iv) Develop new algorithms supporting high-level electron structure calculation of reaction mechanisms (e.g. proton exchange reactions, e.g., in partially hydrated mineral surfaces). With its special emphasis on developing new advanced simulation methodology this research addresses BES needs in high performance computing with a comprehensive focus on unraveling complexity at mineral/fluid interfaces and in disordered materials. Development emphasis is on first principle simulations (forces calculated directly from electronic Schrödinger equation), providing parameter free predictions applicable to a wide range of temperature, pressure and compositions (TPX). The program provides coworkers and the greater EMSL and geochemical community with innovative massively parallel simulation methods required for geochemical applications. In addition, this project in collaboration with P.G. Tratnyek will implement a more transparent pathway modeling “sandbox” using open source tools. NWChem combined with the advanced Arrows workflow will be used to carry out the electronic structure calculations.
Project Details
Start Date
2016-11-09
End Date
2019-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Co-Investigator(s)
Team Members
Related Publications
Bylaska E.J., and K.M. Rosso. 2018. "Corresponding Orbitals Derived from Periodic Bloch States for Electron Transfer Calculations of Transition Metal Oxides." Journal of Chemical Theory and Computation 14, no. 8:4416-4426. PNNL-SA-130874. doi:10.1021/acs.jctc.7b01180
Chen Y, EJ Bylaska, and JH Weare. 2016. "1St Principle Estimation of Geochemically Important Transition Metal Oxide Properties: Structure and Dynamics of the Bulk, Surface and Mineral/Aqueous Fluid Interface." Journal of Molecular Modeling 107-149. doi:10.1002/9781118845226.ch4
Chen Y, EJ Bylaska, and JH Weare. 2017. "Weakly bound water structure, bond valence saturation and water dynamics at the Geothite 100 surface/aqueous interface: Ab initio dynamical simulations." Geochemical Transactions 18:Article No. 3. doi:10.1186/s12932-017-0040-5
Kerisit SN, EJ Bylaska, S Massey, ME McBriarty, and ES Ilton. 2016. "Ab Initio Molecular Dynamics of Uranium Incorporated in Goethite (?-FeOOH): Interpretation of X-Ray Absorption Spectroscopy of Trace Polyvalent Metals." Inorganic Chemistry 55(22):11736–11746. doi:10.1021/acs.inorgchem.6b01773
McBriarty ME, JA Soltis, SN Kerisit, O Qafoku, ME Bowden, EJ Bylaska, JJ De Yoreo, and ES Ilton. 2017. "Trace Uranium Partitioning in a Multi-Phase Nano-FeOOH System." Environmental Science & Technology 51(9):4970-4977. doi:10.1021/acs.est.7b00432
Nguyen T, P Cicotti, EJ Bylaska, D Quinlan, and SB Baden. 2017. "Automatic Translation of MPI Source into a Latency-tolerant, Data-driven Form." Journal of Parallel and Distributed Computing 106:1-13. doi:10.1016/j.jpdc.2017.02.009
Pavitt AS, EJ Bylaska, and PG Tratnyek. 2017. "Oxidation Potentials of Phenols and Anilines: Correlation Analysis of Electrochemical and Theoretical Values." Royal Society of Chemistry 19(3):339-349. doi:10.1039/C6EM00694A
Tratnyek PG, EJ Bylaska, and EJ Weber. 2017. "In Silico Environmental Chemical Science: Properties and Processes From Statistical and Computational Modelling." Environmental Science Processes & Impacts 19(3):188-202. doi:10.1039/c7em00053g