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Title: Quantum dynamical study of the O({sup 1}D) + CH{sub 4} → CH{sub 3} + OH atmospheric reaction

Time independent quantum mechanical (TIQM) scattering calculations have been carried out for the O({sup 1}D) + CH{sub 4}(X{sup 1}A{sub 1}) → CH{sub 3}(X{sup 2}A{sub 2}″) + OH(X{sup 2}Π) atmospheric reaction, using an ab initio ground potential energy surface where the CH{sub 3} group is described as a pseudo-atom. Total and state-to-state reaction probabilities for a total angular momentum J = 0 have been determined for collision energies up to 0.5 eV. The vibrational and rotational state OH product distributions show no specific behavior. The rate coefficient has been calculated by means of the J-shifting approach in the 10–500 K temperature range and slightly depends on T at ordinary temperatures (as expected for a barrierless reaction). Quantum effects do not influence the vibrational populations and rate coefficient in an important way, and a rather good agreement has been found between the TIQM results and the quasiclassical trajectory and experimental ones. This reinforces somewhat the reliability of the pseudo-triatomic approach under the reaction conditions explored.
Authors:
; ;  [1] ;  [2] ;  [3] ;  [4] ;  [4] ;  [5]
  1. Laboratoire de Physique Atomique et Moléculaire et Applications, Département de Physique, Faculté des Sciences, Université Tunis-El Manar, 1060 Tunis (Tunisia)
  2. Institut de Chimie des Milieux et des Matériaux de Poitiers, UMR CNRS 6503, Université de Poitiers, 86022 Poitiers Cedex (France)
  3. Departament de Química Física and IQTC, Universitat de Barcelona, C/Martí i Franqués 1, 08028 Barcelona (Spain)
  4. Laboratoire Interdisciplinaire Carnot de Bourgogne, UMR CNRS 6303, Université de Bourgogne, 21078 Dijon Cedex (France)
  5. (France)
Publication Date:
OSTI Identifier:
22311299
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 140; Journal Issue: 24; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; ANGULAR MOMENTUM; ATOMS; COLLISIONS; METHANE; POTENTIAL ENERGY; QUANTUM MECHANICS; ROTATIONAL STATES; SCATTERING; SURFACES; TEMPERATURE RANGE