Resonant nonlinear spectroscopy in strong fields

Abstract

A method is presented to describe multiple resonant nonlinear spectra in the presence of strong laser fields. The Liouville equation for the d. operator of the mol. system is transformed to a time-independent linear equation system. This can be easily solved rigorously by numerical methods or, after partitioning into a strong-field part and a perturbation, the soln. can be obtained anal. by a novel perturbative approach. The results account for power broadening. Rabi splitting of signals, and power-induced extra resonances, the latter being related to the pure dephasing-induced resonances in the weak-field limit. The method can be applied to a large no. of multiple resonant nonlinear spectroscopies, esp. CARS, CSRS, coherent Rayleigh scattering and sum- or difference-frequency generation.