Simulation of femtosecond time-resolved four-wave mixing experiments on I2

Abstract

Quantum calculations on time-resolved coherent spectroscopy of gas-phase I2 samples are presented. The total polarization induced in the molecules depends on the delay-time between the applied laser pulses. Different contributions reflect the nuclear dynamics in the ground or an excited electronic state. Dependent on the pulse delay-time on one hand and the wavelengths employed on the other, the signal reflects dynamics in a single or in both electronic states. In the case that several initially populated vibrational states contribute to the signal, special care has to be taken of the experimental detection process.