Coherent control of the molecular iodine vibrational dynamics by chirped femtosecond light pulses: theoretical simulation of the pump-probe experiment Original Research Article

Theory of the pump-probe femtosecond experiment response is revisited for diatomic molecules with a special emphasis on the role of phase characteristics of pump and probe light pulses. Theory is used for numerical simulation of the previously reported experimental results for I2 at different chirps of pump and probe pulses Experimentally obtained phase characteristics of the pulses were used in this simulation. Satisfactory agreement between the theory and experiment is obtained both for the shape of the pump-probe experiment signal and for its variation with varying pulse chirps. Calculations confirm previous conclusions about the important effect of the pump-pulse chirp on initial localisation of the wave packet and its subsequent evolution.