Bd. Fainberg, NONPERTURBATIVE ANALYTIC APPROACH TO THE INTERACTION OF INTENSE ULTRASHORT CHIRPED PULSES WITH MOLECULES IN SOLUTION - PICTURE OF MOVING POTENTIALS, The Journal of chemical physics, 109(11), 1998, pp. 4523-4532
A nonperturbative analytic approach to the problem of the interaction
of high-power chirped ultrashort pulses with a molecular system couple
d 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 qu
alitatively with the experimental results by Shank et al. The theory n
aturally leads to the picture of ''moving'' potentials which are ''pho
tonic replications'' of the ground and excited electronic states. An e
lectronic optical transition induced by chirped pulses can be consider
ed as an electron transfer reaction between a ''moving photonic replic
ation'' and the corresponding term occurring at their instantaneous in
tersection. This clear picture explains not only the main features of
the behavior of the excited state population as a function of the chir
p rate, but fine details of it as well. (C) 1998 American Institute of
Physics.