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Mode specific dynamics of the H2 + CH3 → H + CH4 reaction studied using quasi-classical trajectory and eight-dimensional quantum dynamics methods

Journal Article · · Journal of Chemical Physics
DOI:https://doi.org/10.1063/1.4933240· OSTI ID:1469566
 [1];  [2];  [3];  [4];  [3];  [2]
  1. Key Laboratory of Magnetic Resonance in Biological Systems, Wuhan (China). National Center for Magnetic Resonance in Wuhan, State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, Wuhan Institute of Physics and Mathematics, Chinese Academy of Sciences; Hubei University for Nationalities (China). School of Chemical and Environmental Engineering; Key Laboratory of Magnetic Resonance in Biological Systems, Chinese Academy of Sciences, Wuhan 430071, China
  2. Univ. of New Mexico, Albuquerque, NM (United States). Department of Chemistry and Chemical Biology
  3. Key Laboratory of Magnetic Resonance in Biological Systems, Wuhan (China). National Center for Magnetic Resonance in Wuhan, State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, Wuhan Institute of Physics and Mathematics, Chinese Academy of Sciences
  4. Nanyang Technological University (Singapore). Division of Chemistry and Biological Chemistry, School of Physical and Mathematical Sciences
+ Show Author Affiliations
In this work, an eight-dimensional quantum dynamical model is proposed and applied to the title reaction. The reaction probabilities and integral cross sections have been determined for both the ground and excited vibrational states of the two reactants. The results indicate that the H2 stretching and CH3 umbrella modes, along with the translational energy, strongly promote the reactivity, while the CH3 symmetric stretching mode has a negligible effect. The observed mode specificity is confirmed by full-dimensional quasi-classical trajectory calculations. Lastly, the mode specificity can be interpreted by the recently proposed sudden vector projection model, which attributes the enhancement effects of the reactant modes to their strong couplings with the reaction coordinate at the transition state.
Research Organization:
Univ. of New Mexico, Albuquerque, NM (United States)
Sponsoring Organization:
USDOE
Grant/Contract Number:
FG02-05ER15694
OSTI ID:
1469566
Alternate ID(s):
OSTI ID: 1224229
OSTI ID: 22493132
Journal Information:
Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 15 Vol. 143; ISSN JCPSA6; ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English

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Cited By (3)

Full dimensional quantum mechanical calculations of the reaction probability of the H + NH 3 collision based on a mixed Jacobi and Radau description journal May 2019
Counter-propagating wave packets in the quantum transition state approach to reactive scattering journal May 2019
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