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First principles-based multiscale atomistic methods for input into first principles nonequilibrium transport across interfaces

Cheng, Tao and Jaramillo-Botero, Andres and An, Qi and Ilyin, Daniil V. and Naserifar, Saber and Goddard, William A., III (2019) First principles-based multiscale atomistic methods for input into first principles nonequilibrium transport across interfaces. Proceedings of the National Academy of Sciences of the United States of America, 116 (37). pp. 18193-18201. ISSN 0027-8424. PMCID PMC6744898. doi:10.1073/pnas.1800035115.

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This issue of PNAS features “nonequilibrium transport and mixing across interfaces,” with several papers describing the nonequilibrium coupling of transport at interfaces, including mesoscopic and macroscopic dynamics in fluids, plasma, and other materials over scales from microscale to celestial. Most such descriptions describe the materials in terms of the density and equations of state rather than specific atomic structures and chemical processes. It is at interfacial boundaries where such atomistic information is most relevant. However, there is not yet a practical way to couple these phenomena with the atomistic description of chemistry. The starting point for including such information is the quantum mechanics (QM). However, practical QM calculations are limited to a hundred atoms for dozens of picoseconds, far from the scales required to inform the continuum level with the proper atomistic description. To bridge this enormous gap, we need to develop practical methods to extend the scale of the atomistic simulation by several orders of magnitude while retaining the level of QM accuracy in describing the chemical process. These developments would enable continuum modeling of turbulent transport at interfaces to incorporate the relevant chemistry. In this perspective, we will focus on recent progress in accomplishing these extensions in first principles-based atomistic simulations and the strategies being pursued to increase the accuracy of very large scales while dramatically decreasing the computational effort.

Item Type:Article
Related URLs:
URLURL TypeDescription CentralArticle
Cheng, Tao0000-0003-4830-177X
Jaramillo-Botero, Andres0000-0003-2844-0756
An, Qi0000-0003-4838-6232
Ilyin, Daniil V.0000-0003-3534-771X
Naserifar, Saber0000-0002-1069-9789
Goddard, William A., III0000-0003-0097-5716
Additional Information:© 2018 National Academy of Sciences. Published under the PNAS license. Edited by Katepalli R. Sreenivasan, New York University, New York, NY, and approved June 25, 2018 (received for review January 2, 2018). Published ahead of print August 3, 2018. The work reported here on carbon dioxide reduction was supported by the Joint Center for Artificial Photosynthesis, a US Department of Energy (DOE) Energy Innovation Hub, which is supported through Office of Science of the DOE Award DE-SC0004993. The work on PQEq and polarizable reactive force field (ReaxPQ) was supported as part of the Computational Materials Sciences Program funded by DOE, Office of Science, Basic Energy Sciences Award DE-SC00014607 (program manager James Davenport). Other work on ReaxPQ for fuel cells was supported by National Science Foundation Grant CBET 1512759 (program manager Robert McCabe) and the new research using RexPoN is being continued with support from Office of Navel Research (N00014-18-1-2155). The computational resources are from Extreme Science and Engineering Discovery Environment, which is supported by National Science Foundation Grant ACI-1548562. Author contributions: W.A.G. designed research; T.C., A.J.-B., Q.A., D.V.I., and S.N. performed research; and T.C., A.J.-B., Q.A., D.V.I., S.N., and W.A.G. wrote the paper. This article is a PNAS Direct Submission. The authors declare no conflict of interest.
Funding AgencyGrant Number
Joint Center for Artificial Photosynthesis (JCAP)UNSPECIFIED
Department of Energy (DOE)DE-SC0004993
Department of Energy (DOE)DE-SC00014607
Office of Naval Research (ONR)N00014-18-1-2155
Subject Keywords:quantum mechanics; reactive force fields; electron force field; molecular dynamics; multiscale simulation
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Issue or Number:37
PubMed Central ID:PMC6744898
Record Number:CaltechAUTHORS:20180803-131623344
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Official Citation:First principles-based multiscale atomistic methods for input into first principles nonequilibrium transport across interfaces. Tao Cheng, Andres Jaramillo-Botero, Qi An, Daniil V. Ilyin, Saber Naserifar, William A. Goddard. Proceedings of the National Academy of Sciences Sep 2019, 116 (37) 18193-18201; DOI: 10.1073/pnas.1800035115
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:88572
Deposited By: Tony Diaz
Deposited On:03 Aug 2018 20:36
Last Modified:02 Mar 2022 00:42

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