Time-Resolved Photoelectron Spectra of CS sub(2): Dynamics at Conical Intersections

We report results of the application of a fully ab initio approach for simulating time-resolved molecular-frame photoelectron angular distributions around conical intersections in CS sub(2). The technique employs wave packet densities obtained with the multiple spawning method in conjunction with geometry- and energy-dependent photoionization matrix elements. The robust agreement of these results with measured molecular-frame photoelectron angular distributions for CS sub(2) demonstrates that this technique can successfully elucidate, and disentangle, the underlying nuclear and photoionization dynamics around conical intersections in polyatomic molecules.