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Title: Communication: Rate coefficients of the H + CH{sub 4} → H{sub 2} + CH{sub 3} reaction from ring polymer molecular dynamics on a highly accurate potential energy surface

Abstract

The ring polymer molecular dynamics (RPMD) calculations are performed to calculate rate constants for the title reaction on the recently constructed potential energy surface based on permutation invariant polynomial (PIP) neural-network (NN) fitting [J. Li et al., J. Chem. Phys. 142, 204302 (2015)]. By inspecting convergence, 16 beads are used in computing free-energy barriers at 300 K ≤ T ≤ 1000 K, while different numbers of beads are used for transmission coefficients. The present RPMD rates are in excellent agreement with quantum rates computed on the same potential energy surface, as well as with the experimental measurements, demonstrating further that the RPMD is capable of producing accurate rates for polyatomic chemical reactions even at rather low temperatures.

Authors:
;
Publication Date:
OSTI Identifier:
22489548
Resource Type:
Journal Article
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 143; Journal Issue: 10; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0021-9606
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; CHEMICAL REACTIONS; FREE ENERGY; HYDROGEN; METHANE; MOLECULAR DYNAMICS METHOD; NEURAL NETWORKS; POLYMERS; POLYNOMIALS; POTENTIAL ENERGY; REACTION KINETICS; SURFACES

Citation Formats

Meng, Qingyong, Chen, Jun, and Zhang, Dong H., E-mail: zhangdh@dicp.ac.cn. Communication: Rate coefficients of the H + CH{sub 4} → H{sub 2} + CH{sub 3} reaction from ring polymer molecular dynamics on a highly accurate potential energy surface. United States: N. p., 2015. Web. doi:10.1063/1.4930860.
Meng, Qingyong, Chen, Jun, & Zhang, Dong H., E-mail: zhangdh@dicp.ac.cn. Communication: Rate coefficients of the H + CH{sub 4} → H{sub 2} + CH{sub 3} reaction from ring polymer molecular dynamics on a highly accurate potential energy surface. United States. https://doi.org/10.1063/1.4930860
Meng, Qingyong, Chen, Jun, and Zhang, Dong H., E-mail: zhangdh@dicp.ac.cn. 2015. "Communication: Rate coefficients of the H + CH{sub 4} → H{sub 2} + CH{sub 3} reaction from ring polymer molecular dynamics on a highly accurate potential energy surface". United States. https://doi.org/10.1063/1.4930860.
@article{osti_22489548,
title = {Communication: Rate coefficients of the H + CH{sub 4} → H{sub 2} + CH{sub 3} reaction from ring polymer molecular dynamics on a highly accurate potential energy surface},
author = {Meng, Qingyong and Chen, Jun and Zhang, Dong H., E-mail: zhangdh@dicp.ac.cn},
abstractNote = {The ring polymer molecular dynamics (RPMD) calculations are performed to calculate rate constants for the title reaction on the recently constructed potential energy surface based on permutation invariant polynomial (PIP) neural-network (NN) fitting [J. Li et al., J. Chem. Phys. 142, 204302 (2015)]. By inspecting convergence, 16 beads are used in computing free-energy barriers at 300 K ≤ T ≤ 1000 K, while different numbers of beads are used for transmission coefficients. The present RPMD rates are in excellent agreement with quantum rates computed on the same potential energy surface, as well as with the experimental measurements, demonstrating further that the RPMD is capable of producing accurate rates for polyatomic chemical reactions even at rather low temperatures.},
doi = {10.1063/1.4930860},
url = {https://www.osti.gov/biblio/22489548}, journal = {Journal of Chemical Physics},
issn = {0021-9606},
number = 10,
volume = 143,
place = {United States},
year = {Mon Sep 14 00:00:00 EDT 2015},
month = {Mon Sep 14 00:00:00 EDT 2015}
}