Full-dimensional and reduced-dimensional calculations of initial state-selected reaction probabilities studying the H + CH4 -> H-2 + CH3 reaction on a neural network PES

Welsch R, Manthe U (2015)
The Journal of Chemical Physics 142(6): 064309.

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Zeitschriftenaufsatz | Veröffentlicht | Englisch
Abstract / Bemerkung
Initial state-selected reaction probabilities of the H + CH4 -> H-2 + CH3 reaction are calculated in full and reduced dimensionality on a recent neural network potential [X. Xu, J. Chen, and D. H. Zhang, Chin. J. Chem. Phys. 27, 373 (2014)]. The quantum dynamics calculation employs the quantum transition state concept and the multi-layer multi-configurational time-dependent Hartree approach and rigorously studies the reaction for vanishing total angular momentum (J = 0). The calculations investigate the accuracy of the neutral network potential and study the effect resulting from a reduced-dimensional treatment. Very good agreement is found between the present results obtained on the neural network potential and previous results obtained on a Shepard interpolated potential energy surface. The reduced-dimensional calculations only consider motion in eight degrees of freedom and retain the C-3v symmetry of the methyl fragment. Considering reaction starting from the vibrational ground state of methane, the reaction probabilities calculated in reduced dimensionality are moderately shifted in energy compared to the full-dimensional ones but otherwise agree rather well. Similar agreement is also found if reaction probabilities averaged over similar types of vibrational excitation of the methane reactant are considered. In contrast, significant differences between reduced and full-dimensional results are found for reaction probabilities starting specifically from symmetric stretching, asymmetric (f(2)-symmetric) stretching, or e-symmetric bending excited states of methane. (C) 2015 AIP Publishing LLC.
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Zeitschriftentitel
The Journal of Chemical Physics
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142
Zeitschriftennummer
6
Artikelnummer
064309
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Welsch R, Manthe U. Full-dimensional and reduced-dimensional calculations of initial state-selected reaction probabilities studying the H + CH4 -> H-2 + CH3 reaction on a neural network PES. The Journal of Chemical Physics. 2015;142(6): 064309.
Welsch, R., & Manthe, U. (2015). Full-dimensional and reduced-dimensional calculations of initial state-selected reaction probabilities studying the H + CH4 -> H-2 + CH3 reaction on a neural network PES. The Journal of Chemical Physics, 142(6), 064309. doi:10.1063/1.4906825
Welsch, R., and Manthe, U. (2015). Full-dimensional and reduced-dimensional calculations of initial state-selected reaction probabilities studying the H + CH4 -> H-2 + CH3 reaction on a neural network PES. The Journal of Chemical Physics 142:064309.
Welsch, R., & Manthe, U., 2015. Full-dimensional and reduced-dimensional calculations of initial state-selected reaction probabilities studying the H + CH4 -> H-2 + CH3 reaction on a neural network PES. The Journal of Chemical Physics, 142(6): 064309.
R. Welsch and U. Manthe, “Full-dimensional and reduced-dimensional calculations of initial state-selected reaction probabilities studying the H + CH4 -> H-2 + CH3 reaction on a neural network PES”, The Journal of Chemical Physics, vol. 142, 2015, : 064309.
Welsch, R., Manthe, U.: Full-dimensional and reduced-dimensional calculations of initial state-selected reaction probabilities studying the H + CH4 -> H-2 + CH3 reaction on a neural network PES. The Journal of Chemical Physics. 142, : 064309 (2015).
Welsch, Ralph, and Manthe, Uwe. “Full-dimensional and reduced-dimensional calculations of initial state-selected reaction probabilities studying the H + CH4 -> H-2 + CH3 reaction on a neural network PES”. The Journal of Chemical Physics 142.6 (2015): 064309.

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