Nonperturbative simulation of pump–probe spectra for electron transfer reactions in the condensed phase

A new method is proposed for simulating time-resolved nonlinear optical spectra associated with electron transfer (ET) reactions in the condensed phase. The method is based on a combination of the nonperturbative approach to describe nonlinear optical signals and the self-consistent hybrid method to simulate quantum dynamics for large systems. The potential of the method is illustrated by applications to several models of ET reactions in solution. Furthermore, the manifestation of ET dynamics and nuclear dynamics in transient absorption spectra is discussed in some detail.