The role of the transition state in polyatomic reactions: Initial state-selected reaction probabilities of the H + CH4 -> H-2 + CH3 reaction

Welsch R, Manthe U (2014)
The Journal of Chemical Physics 141(17): 174313.

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DOI
Autor*in
Welsch, RalphUniBi; Manthe, UweUniBi
Einrichtung
Fakultät für Chemie > Theoretische Chemie
Abstract / Bemerkung
Full-dimensional calculations of initial state-selected reaction probabilities on an accurate ab initio potential energy surface (PES) have been communicated recently [R. Welsch and U. Manthe, J. Chem. Phys. 141, 051102 (2014)]. These calculations use the quantum transition state concept, the multi-layer multi-configurational time-dependent Hartree approach, and graphics processing units to speed up the potential evaluation. Here further results of these calculations and an extended analysis are presented. State-selected reaction probabilities are given for many initial ro-vibrational states. The role of the vibrational states of the activated complex is analyzed in detail. It is found that rotationally cold methane mainly reacts via the ground state of the activated complex while rotationally excited methane mostly reacts via H-H-CH3-bending excited states of the activated complex. Analyzing the different contributions to the reactivity of the vibrationally states of methane, a complex pattern is found. Comparison with initial state-selected reaction probabilities computed on the semi-empirical Jordan-Gilbert PES reveals the dependence of the results on the specific PES. (C) 2014 AIP Publishing LLC.
Erscheinungsjahr
2014
Zeitschriftentitel
The Journal of Chemical Physics
Band
141
Ausgabe
17
Art.-Nr.
174313
ISSN
0021-9606
eISSN
1089-7690
Page URI
https://pub.uni-bielefeld.de/record/2710542

Zitieren

Welsch R, Manthe U. The role of the transition state in polyatomic reactions: Initial state-selected reaction probabilities of the H + CH4 -> H-2 + CH3 reaction. The Journal of Chemical Physics. 2014;141(17): 174313.
Welsch, R., & Manthe, U. (2014). The role of the transition state in polyatomic reactions: Initial state-selected reaction probabilities of the H + CH4 -> H-2 + CH3 reaction. The Journal of Chemical Physics, 141(17), 174313. doi:10.1063/1.4900735
Welsch, Ralph, and Manthe, Uwe. 2014. “The role of the transition state in polyatomic reactions: Initial state-selected reaction probabilities of the H + CH4 -> H-2 + CH3 reaction”. The Journal of Chemical Physics 141 (17): 174313.
Welsch, R., and Manthe, U. (2014). The role of the transition state in polyatomic reactions: Initial state-selected reaction probabilities of the H + CH4 -> H-2 + CH3 reaction. The Journal of Chemical Physics 141:174313.
Welsch, R., & Manthe, U., 2014. The role of the transition state in polyatomic reactions: Initial state-selected reaction probabilities of the H + CH4 -> H-2 + CH3 reaction. The Journal of Chemical Physics, 141(17): 174313.
R. Welsch and U. Manthe, “The role of the transition state in polyatomic reactions: Initial state-selected reaction probabilities of the H + CH4 -> H-2 + CH3 reaction”, The Journal of Chemical Physics, vol. 141, 2014, : 174313.
Welsch, R., Manthe, U.: The role of the transition state in polyatomic reactions: Initial state-selected reaction probabilities of the H + CH4 -> H-2 + CH3 reaction. The Journal of Chemical Physics. 141, : 174313 (2014).
Welsch, Ralph, and Manthe, Uwe. “The role of the transition state in polyatomic reactions: Initial state-selected reaction probabilities of the H + CH4 -> H-2 + CH3 reaction”. The Journal of Chemical Physics 141.17 (2014): 174313.

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