Analysis of cross peaks in two-dimensional electronic photon-echo spectroscopy for simple models with vibrations and dissipation

Abstract

The recently developed efficient method for the calculation of four-wave mixing signals [M. F. Gelin et al., J. Chem. Phys. 123, 164112 (2005)] is employed for the calculation of two-dimensional electronic photon-echo spectra. The effect of the explicit treatment of vibrations coupled to the electronic transitions is systematically analyzed. The impact of pulse durations, optical dephasing, and temperature on the spectra is investigated. The study aims at an understanding of the mechanisms which may give rise to cross peaks in the two-dimensional electronic spectra and at clarifying the conditions of their detection.