Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 116, Issue 37, Pages 18202-18208Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1701383115
Keywords
reaction kinetics; ReaxFF reactive force field; reactive molecular dynamics; RMD2Kin; ReaxMD2Kin
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Funding
- US Department of Energy, Office of Energy Efficiency and Renewable Energy, Advanced Manufacturing Office Next Generation RD Projects [DE-AC07-05ID14517]
- Office of Naval Research [N00014-12-1-0538]
- California Institute of Technology Toni and Bob Perpall Summer Undergraduate Research Fellowship
- California Institute of Technology Ernest H Swift Summer Undergraduate Research Fellowship
- Australian Government
- Government of Western Australia
- National Science Foundation [ACI-1548562]
- University of Western Australia
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This paper presents our vision of how to use in silico approaches to extract the reaction mechanisms and kinetic parameters for complex condensed-phase chemical processes that underlie important technologies ranging from combustion to chemical vapor deposition. The goal is to provide an analytic description of the detailed evolution of a complex chemical system from reactants through various intermediates to products, so that one could optimize the efficiency of the reactive processes to produce the desired products and avoid unwanted side products. We could start with quantum mechanics (QM) to ensure an accurate description; however, to obtain useful kinetics we need to average over similar to 10-nm spatial scales for similar to 1 ns, which is prohibitively impractical with QM. Instead, we use the reactive force field (ReaxFF) trained to fit QM to carry out the reactive molecular dynamics (RMD). We focus here on showing that it is practical to extract from such RMD the reaction mechanisms and kinetics information needed to describe the reactions analytically. This analytic description can then be used to incorporate the correct reaction chemistry from the QM/ReaxFF atomistic description into larger-scale simulations of similar to 10 nm to micrometers to millimeters to meters using analytic approaches of computational fluid dynamics and/or continuum chemical dynamics. In the paper we lay out the strategy to extract the mechanisms and rate parameters automatically without the necessity of knowing any details of the chemistry. We consider this to be a proof of concept. We refer to the process as RMD2Kin (reactive molecular dynamics to kinetics) for the general approach and as ReaxMD2Kin (ReaxFF molecular dynamics to kinetics) for QM-ReaxFF-based reaction kinetics.
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