Time-resolved photoelectron spectroscopy of molecular dissociation: Classical trajectory versus quantum wave-placket calculations

摘要

We present a simulation of ultrafast pump-probe photoelectron specroscopy based on a classical treatment of the nuclear motion. A comparison with quantum mechanical wave-packet results shows that in the case of the direct dissociation of H_2O in its A ~1B_1 electronic state this method produces extremely accurate results. The energy distribution of the photoelectrons recorded as a function of the pump-probe delay reflects the dissociation process, which takes place within only a few femtoseconds.