Ring Polymer Molecular Dynamics Calculations of Thermal Rate Constants for the O([superscript 3]P) + CH[subscript 4] → OH + CH[subscript 3] Reaction: Contributions of Quantum Effects
Author(s)
Li, Yongle
Suleimanov, Yury V.
Yang, Minghui
Green, William H.
Guo, Hua
Date Issued
December 2012
Journal
The Journal of Physical Chemistry Letters
Publisher
American Chemical Society (ACS)
Citation
Li, Yongle, Yury V. Suleimanov, Minghui Yang, William H. Green, and Hua Guo. “Ring Polymer Molecular Dynamics Calculations of Thermal Rate Constants for the O([superscript 3]P) + CH[subscript 4] → OH + CH[subscript 3] Reaction: Contributions of Quantum Effects.” The Journal of Physical Chemistry Letters 4, no. 1 (January 3, 2013): 48–52.
Version
Author's final manuscript
Abstract
The thermal rate constant of the O([superscript 3]P) + CH[subscript 4] → OH + CH[subscript 3] reaction is investigated with ring polymer molecular dynamics on a full-dimensional potential energy surface. Good agreement with experimental and full-dimensional quantum multiconfiguration time-dependent Hartree results between 300 and 1500 K was obtained. It is shown that quantum effects, for example, tunneling and zero-point energy, can be effectively and efficiently included in this path-integral based approach implemented with classical trajectories. Convergence with respect to the number of beads is rapid, suggesting wide applicability for other reactions involving polyatomic molecules.
MIT Department
Massachusetts Institute of Technology. Department of Chemical Engineering
Terms of Use
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Persistent DSpace Link
DOI of Published Version
https://doi.org/10.1021/jz3019513
