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Title: Calculation of state-to-state differential and integral cross sections for atom-diatom reactions with transition-state wave packets

A recently proposed transition-state wave packet method [R. Welsch, F. Huarte-LarraƱaga, and U. Manthe, J. Chem. Phys. 136, 064117 (2012)] provides an efficient and intuitive framework to study reactive quantum scattering at the state-to-state level. It propagates a few transition-state wave packets, defined by the eigenfunctions of the low-rank thermal flux operator located near the transition state, into the asymptotic regions of the reactant and product arrangement channels separately using the corresponding Jacobi coordinates. The entire S-matrix can then be assembled from the corresponding flux-flux cross-correlation functions for all arrangement channels. Since the transition-state wave packets can be defined in a relatively small region, its transformation into either the reactant or product Jacobi coordinates is accurate and efficient. Furthermore, the grid/basis for the propagation, including the maximum helicity quantum number K, is much smaller than that required in conventional wave packet treatments of state-to-state reactive scattering. This approach is implemented for atom-diatom reactions using a time-dependent wave packet method and applied to the H + D{sub 2} reaction with all partial waves. Excellent agreement with benchmark integral and differential cross sections is achieved.
Authors:
 [1] ;  [2] ;  [1] ;  [3]
  1. Center for Theoretical and Computational Chemistry, and State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023 (China)
  2. (United States)
  3. Department of Chemistry and Chemical Biology, University of New Mexico, Albuquerque, New Mexico 87131 (United States)
Publication Date:
OSTI Identifier:
22420055
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:
97 MATHEMATICAL METHODS AND COMPUTING; ATOMS; CORRELATION FUNCTIONS; DIFFERENTIAL CROSS SECTIONS; EIGENFUNCTIONS; INTEGRAL CROSS SECTIONS; INTEGRALS; PARTIAL WAVES; SCATTERING; TIME DEPENDENCE; WAVE PACKETS