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Title: Communication: Direct comparison between theory and experiment for correlated angular and product-state distributions of the ground-state and stretching-excited O({sup 3}P) + CH{sub 4} reactions

Motivated by a recent experiment [H. Pan and K. Liu, J. Chem. Phys. 140, 191101 (2014)], we report a quasiclassical trajectory study of the O({sup 3}P) + CH{sub 4}(v{sub k} = 0, 1) → OH + CH{sub 3} [k = 1 and 3] reactions on an ab initio potential energy surface. The computed angular distributions and cross sections correlated to the OH(v = 0, 1) + CH{sub 3}(v = 0) coincident product states can be directly compared to experiment for O + CH{sub 4}(v{sub 3} = 0, 1). Both theory and experiment show that the ground-state reaction is backward scattered, whereas the angular distributions shift toward sideways and forward directions upon antisymmetric stretching (v{sub 3}) excitation of the reactant. Theory predicts similar behavior for the O + CH{sub 4}(v{sub 1} = 1) reaction. The simulations show that stretching excitation enhances the reaction up to about 15 kcal/mol collision energy, whereas the O + CH{sub 4}(v{sub k} = 1) reactions produce smaller cross sections for OH(v = 1) + CH{sub 3}(v = 0) than those of O + CH{sub 4}(v = 0) → OH(v = 0) + CH{sub 3}(v = 0). The former finding agrees with experiment and the latter awaitsmore » for confirmation. The computed cold OH rotational distributions of O + CH{sub 4}(v = 0) are in good agreement with experiment.« less
Authors:
 [1]
  1. Laboratory of Molecular Structure and Dynamics, Institute of Chemistry, Eötvös University, H-1518, P. O. Box 32, Budapest 112 (Hungary)
Publication Date:
OSTI Identifier:
22420121
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 140; Journal Issue: 23; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; COLLISIONS; COMPARATIVE EVALUATIONS; CROSS SECTIONS; EXCITATION; GROUND STATES; METHANE; POTENTIAL ENERGY; SIMULATION