Resonant Femtosecond Stimulated Raman Spectra: Theory and Simulations

We present a description of resonant femtosecond stimulated Raman spectra, which is based on the solution of the nonperturbative equation of motion of the chromophore in the laser fields. The theory is applicable for arbitrary shapes and durations of the Raman pulses, accounts for excited-state absorption, and describes nonstationary preparation of the system by an actinic pulse. The method is illustrated by the calculation of femtosecond stimulated Raman spectra of a model system with a conical intersection.