COHERENCE, TRANSIENTS, AND INTERFERENCE IN PHOTODISSOCIATION WITH ULTRASHORT PULSES

We summarize recent theoretical studies that were carried out at the University of California, Santa Barbara, that are pertinent to photodissociation with femtosecond pulses. The emphasis is on describing new phenomena that have been proved to exist by exact calculations and on explaining them in simple qualitative terms. We are concerned with (a) the connection between the laser-induced fluorescence signal generated by the pumpprobe experiments and the dynamics of photodissociation, (b) the coherence of the state that is prepared by the pump and the pump’s ability to generate beats in the laser-induced fluorescence signal, (c) the time evolution of the final-state distribution after excitation by the pump, (d) the properties of the short-time transients that are generated by off-resonance excitation, and (e) the role of interference in modifying the photodissociation yield when the molecule is able to absorb the photon from one of two different pulses. © 1990 Optical Society of America.