We discuss an extension of our formulation of energy- and angle-resolved photoelectron spectra for femtosecond pump-probe ionization of wave packets to nonadiabatically coupled states and present results of its applications to wave packet motion on the ionic (Na+I-) and covalent (NaI) states of sodium iodide. The results of these studies suggest that the energy and angular distributions of these photoelectron spectra provide a useful mapping of the bifurcation of the wave packets through the crossing region and a valuable window on the intramolecular electron transfer occurring between the covalent and ionic states (NaI-->Na+I-). (C) 2003 American Institute of Physics.