Calculating initial-state-selected reaction probabilities from thermal flux eigenstates: a transition-state-based approach.
An approach for the calculation of initial-state-selected reaction probabilities utilizing a transition-state view and the multiconfigurational time-dependent Hartree approach is presented. Using flux correlation functions, wave packets located in the transition-state region are constructed and propagated into the asymptotic region to obtain initial-state-selected reaction probabilities. A complete set of reaction probabilities is obtained from a single set of thermal flux eigenstates. Concepts previously applied with success to the calculation of k(T) or N(E) are transferred to the calculation of state-selected probabilities. The benchmark H+H(2) (J=0) reaction on the LSTH potential-energy surface is used to test the reliability of this approach.
Huarte-Larrañaga
Fermín
F
Centre Especial de Recerca en Química Teòrica, Parc Científic de Barcelona, Josep Samitier 5, 08028 Barcelona, Spain. fhuarte@pcb.ub.es
Manthe
Uwe
U