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

Theory of the pump-probe femtosecond experiment response is revisited for d iatomic molecules with a special emphasis on the role of phase characterist ics of pump and probe light pulses. Theory is used for numerical simulation of the previously reported experimental results for I-2 at different chirp s of pump and probe pulses Experimentally obtained phase characteristics of the pulses were used in this simulation. Satisfactory agreement between th e theory and experiment is obtained both for the shape of the pump-probe ex periment signal and for its variation with varying pulse chirps. Calculatio ns confirm previous conclusions about the important effect of the pump-puls e chirp on initial localisation of the wave packet and its subsequent evolu tion. (C) 1999 Elsevier Science B.V. All rights reserved.