Shannon, RJ, Martínez-Núñez, E, Shalashilin, DV orcid.org/0000-0001-6104-1277 et al. (1 more author) (2021) ChemDyME: Kinetically Steered, Automated Mechanism Generation through Combined Molecular Dynamics and Master Equation Calculations. Journal of Chemical Theory and Computation, 17 (8). pp. 4901-4912. ISSN 1549-9618
Abstract
In many scientific fields, there is an interest in understanding the way in which chemical networks evolve. The chemical networks which researchers focus upon have become increasingly complex, and this has motivated the development of automated methods for exploring chemical reactivity or conformational change in a “black-box” manner, harnessing modern computing resources to automate mechanism discovery. In this work, we present a new approach to automated mechanism generation which couples molecular dynamics and statistical rate theory to automatically find kinetically important reactions and then solve the time evolution of the species in the evolving network. The key to this chemical network mapping through combined dynamics and ME simulation approach is the concept of “kinetic convergence”, whereby the search for new reactions is constrained to those species which are kinetically favorable at the conditions of interest. We demonstrate the capability of the new approach for two systems, a well-studied combustion system and a multiple oxygen addition system relevant to atmospheric aerosol formation.
Metadata
Item Type: | Article |
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Authors/Creators: |
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Copyright, Publisher and Additional Information: | © 2021 American Chemical Society. This is an author produced version of an article, published in Journal of Chemical Theory and Computation. Uploaded in accordance with the publisher's self-archiving policy. |
Dates: |
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Institution: | The University of Leeds |
Academic Units: | The University of Leeds > Faculty of Engineering & Physical Sciences (Leeds) > School of Chemistry (Leeds) > Physical Chemistry (Leeds) |
Depositing User: | Symplectic Publications |
Date Deposited: | 06 Aug 2021 11:04 |
Last Modified: | 20 Jul 2022 00:13 |
Status: | Published |
Publisher: | American Chemical Society |
Identification Number: | 10.1021/acs.jctc.1c00335 |
Open Archives Initiative ID (OAI ID): | oai:eprints.whiterose.ac.uk:176813 |