Coherent nonlinear spectroscopy: from femtosecond dynamics to control.

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.