Transition state theory for laser-driven reactions

摘要

Recent developments in transition state theory brought about by dynamical systems theory are extended to time-dependent systems such as laser-driven reactions.Using time-dependent normal form theory,the authors construct a reaction coordinate with regular dynamics inside the transition region.The conservation of the associated action enables one to extract time-dependent invariant manifolds that act as separatrices between reactive and nonreactive trajectories and thus make it possible to predict the ultimate fate of a trajectory.They illustrate the power of our approach on a driven Henon-Heiles system,which serves as a simple example of a reactive system with several open channels.The present generalization of transition state theory to driven systems will allow one to study processes such as the control of chemical reactions through laser pulses.