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A comparison study of the H + CH4 and H + SiH4 reactions with eight-dimensional quantum dynamics: normal mode versus local mode in the reactant molecule vibration

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Abstract

While molecular vibration of CH4 is well described by the normal-mode paradigm, the local mode picture is more suitable for understanding the SiH4 stretching vibrational motion. To compare the roles of the two types of molecular vibration in reaction dynamics, the H + CH4 → H2 + CH3 and H + SiH4 → H2 + SiH3 reactions have been investigated using an eight-dimensional (8D) quantum dynamics method in which the nonreacting XH3 (X = C, Si) group keeps its C3v symmetry in the reaction. The reaction probabilities, integral cross sections and thermal rate constants in the temperature range of 200–2,000 K were calculated for both reactions. Strong mode specificity was found in both reactions, and the differences were rationalized by the vibrational characteristics of the CH4 and SiH4 reactants.

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Acknowledgments

This work was supported by National Science Foundation of China (Projects No. 21221064 and 21373266 to MY) and US Department of Energy (DE-FG02-05ER15694 to HG).

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Authors and Affiliations

  1. Key Laboratory of Magnetic Resonance in Biological Systems, Wuhan Center for Magnetic Resonance, State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, Wuhan Institute of Physics and Mathematics, Chinese Academy of Sciences, Wuhan, 430071, People’s Republic of China

    Yan Wang & Minghui Yang

  2. School of Chemical and Environmental Engineering, Hubei University for Nationalities, Enshi, 445000, People’s Republic of China

    Yan Wang

  3. Department of Chemistry and Chemical Biology, University of New Mexico, Albuquerque, NM, 87131, USA

    Jun Li & Hua Guo

Authors
  1. Yan Wang
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  2. Jun Li
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  3. Hua Guo
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  4. Minghui Yang
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Corresponding author

Correspondence to Minghui Yang.

Additional information

Dedicated to Professor Guosen Yan and published as part of the special collection of articles celebrating his 85th birthday.

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Wang, Y., Li, J., Guo, H. et al. A comparison study of the H + CH4 and H + SiH4 reactions with eight-dimensional quantum dynamics: normal mode versus local mode in the reactant molecule vibration. Theor Chem Acc 133, 1555 (2014). https://doi.org/10.1007/s00214-014-1555-9

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