Please use this identifier to cite or link to this item:
http://hdl.handle.net/2445/46034
Title: | State-to-state reaction probabilities within the quantum transition state framework |
Author: | Welsch, Ralph Huarte Larrañaga, Fermín Manthe, Uwe |
Keywords: | Teoria quàntica Reaccions químiques Quantum theory Chemical reactions |
Issue Date: | 14-Feb-2012 |
Publisher: | American Institute of Physics |
Abstract: | Rigorous quantum dynamics calculations of reaction rates and initial state-selected reaction probabilities of polyatomic reactions can be efficiently performed within the quantum transition state concept employing flux correlation functions and wave packet propagation utilizing the multi-configurational time-dependent Hartree approach. Here, analytical formulas and a numerical scheme extending this approach to the calculation of state-to-state reaction probabilities are presented. The formulas derived facilitate the use of three different dividing surfaces: two dividing surfaces located in the product and reactant asymptotic region facilitate full state resolution while a third dividing surface placed in the transition state region can be used to define an additional flux operator. The eigenstates of the corresponding thermal flux operator then correspond to vibrational states of the activated complex. Transforming these states to reactant and product coordinates and propagating them into the respective asymptotic region, the full scattering matrix can be obtained. To illustrate the new approach, test calculations study the D + H2(ν, j) → HD(ν′, j′) + H reaction for J = 0. |
Note: | Reproducció del document publicat a: http://dx.doi.org/10.1063/1.3684631 |
It is part of: | Journal of Chemical Physics, 2012, vol. 136, num. 6, p. 064117-1-064117-11 |
URI: | http://hdl.handle.net/2445/46034 |
Related resource: | http://dx.doi.org/10.1063/1.3684631 |
ISSN: | 0021-9606 |
Appears in Collections: | Articles publicats en revistes (Ciència dels Materials i Química Física) |
Files in This Item:
File | Description | Size | Format | |
---|---|---|---|---|
607579.pdf | 1.03 MB | Adobe PDF | View/Open |
Items in DSpace are protected by copyright, with all rights reserved, unless otherwise indicated.