Journal of Chemical Physics, Vol.108, No.12, 4862-4876, 1998
Temporal coherent control in the photoionization of Cs-2 : Theory and experiment
Two identical femtosecond pulses are used to create a coherent superposition of two vibrational wave packets in a bound electronic state of cesium dimers. The oscillations of these two wave packets are further detected after photoionization of the system. Quantum interferences between the two wave packets result in a temporal coherent control of the ionization probability. The interferogram exhibits the following features as a function of the time delay between the two laser pulses : high-frequency oscillation corresponding to Ramsey fringes (at the Bohr frequency of the transition) modulated by a slow envelope corresponding to the oscillations of vibrational wave packets (vibrational recurrences). Here the control parameter is the time delay between the two laser pulses which can be used to control the preparation of a wave packet in a quantum system and monitor its evolution. The detailed theory of this experiment is presented and compared with the pump-probe experiment, The temporal coherent control experiment is performed in the B state of Cs-2, at 768 nm, with 150 fs pulses. We finally analyze quantitatively and discuss the effects of a thermal distribution of initial states on the temporal coherent control signal.
Keywords:WAVE-PACKET DYNAMICS;PHOTOELECTRON ANGULAR-DISTRIBUTIONS;MOLECULAR MULTIPHOTON IONIZATION;FEMTOSECOND LASER-PULSES;TIME-RESOLVED DYNAMICS;PUMP-PROBE EXPERIMENTS;PHASE-LOCKED PULSES;OPTICAL PULSES;QUANTUM-WELLS;DISSOCIATION REACTIONS