COHERENT NONLINEAR SPECTROSCOPY: From Femtosecond Dynamics to Control

Abstract

▪ Abstract  This review focuses on the study of the dynamics of isolated molecules and their control using coherent nonlinear spectroscopic methods. Emphasis is placed on topics such as bound-to-free excitation and the study of concerted elimination reactions, free-to-bound excitation and the study of bimolecular reactions, and bound-to-bound excitation and the study of intramolecular rovibrational dynamics and coherence relaxation. For each case the detailed time-resolved information reveals possible strategies to control the outcome. Experimental results are shown for each of the reactions discussed. The methods discussed include pump-probe and four-wave mixing processes such as transient grating and photon echo spectroscopy. Off-resonance transient-grating experiments are shown to be ideal for the study of ground state dynamics, molecular structure, and the molecular response to strong field excitation.