Interaction of intense chirped pulses with molecules in condensed phase as electron transfer between “moving” potential

Abstract

A nonperturbative analytic approach to the problem of the interaction of high-power chirped pulses with molecular systems: the picture of “moving potentials” (J. Chem. Phys., 109 (1998) 4523) has been generalized to different relaxation times in the ground and in the excited electronic states. The calculation results agree qualitatively with the experimental results by Shank et al. and Bardeen, Wilson et al. 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 occuring at their instantaneous intersection. This clear picture explains even fine details of the behaviour of the excited state population as a function of the chirp rate.