Laser-induced rate processes in gases: Dynamics of polyatomic systems

Abstract

A model is proposed to describe the collision-free dynamics of a polyatomic molecule driven by an intense laser field. The evolution in time of stable and quasistable (chemically reactive) energy level populations driven on and off resonance are given, and analytic estimates are derived for the effects of dynamic power broadening (a–c Stark effect), mode and level degeneracies, and rapid unimolecular decay on the efficiency of laser pumping.