Probing wavepacket dynamics with femtosecond energy- and angle-resolved photoelectron spectroscopy

Femtosecond energy- and angle-resolved pump-probe photoelectron spectra of wavepackets in a double-minimum state of Na_2 are studied. These studies illustrate that a robust description of the photoionization dynamics significantly enhances the utility of time-resolved photoelectron spectroscopy as a probe of wavepackets and of the evolution of electronic structure, particularly in regions of avoided crossings, and that the dependence of these angular distributions on the relative polarizations of the pump and probe lasers can be exploited to monitor molecular alignment.