Three-dimensional quantum theory of triatomic exchange reactions in strong laser fields is presented. Our theory consists of an exact partitioning technique for treating the effects of optical fields on reactive scattering, based on approximate hindered-rotor adiabatic wave functions describing the pure nonradiative events. The method enables computations to be performed for an arbitrary number of field intensities with very little effort beyond that required for a single-intensity computation. Differential and integral cross sections for the H+H2 exchange reaction, involving the ground and first excited electronic states, in the presence of laser fields, are computed. The dependence of reactive nonlinear optical effects, and especially that of "laser catalysis," on laser intensity; the way isolated and overlapping power-broadened resonances affect the optically induced reaction; the role of relative orientation of two incident molecular beams in crossed beams experiments are investigated. The three-dimensional computations confirm our previous expectations, based on a collinear model, that laser catalysis is achievable using only moderately high powered lasers. The above is expected to be true for all reactive systems (of which H + H2 is one) possessing optically allowed stable excited electronic states.
ASJC Scopus subject areas
- Physics and Astronomy(all)
- Physical and Theoretical Chemistry