Nonperturbative analytic approach to the interaction of intense ultrashort chirped pulses with molecules in solution: Picture of “moving” potentials

Abstract

A nonperturbative analytic approach to the problem of the interaction of high-power chirped ultrashort pulses with a molecular system coupled with a dissipative environment has been developed. We considered the model of the Gaussian–Markovian stochastic modulation of the optical transition of a molecule in solution. The calculation results agree qualitatively with the experimental results by Shank et al. The theory naturally leads to the picture of “moving” potentials which are “photonic replications” of the ground and excited electronic states. An electronic optical transition induced by chirped pulses can be considered as an electron transfer reaction between a “moving photonic replication” and the corresponding term occurring at their instantaneous intersection. This clear picture explains not only the main features of the behavior of the excited state population as a function of the chirp rate, but fine details of it as well.