Combining Structural and Spectroscopic Probes of Molecular Dynamics

We combine ultrafast electron diffraction (UED) measurements with time resolved photoelectron spectroscopy (TPRES) measurements of excited state molecular dynamics. Both measurements are compared with trajectory surface hopping calculations of the dynamics, which can produce the measurement observables in both cases. The measurements highlight the non-local dynamics captured by different groups of trajectories in the calculations.~ This is the first time that both structural and spectroscopic measurements are combined with a theory capable of calculating the measurement observables in both cases, and the combination yields an unprecedented view of the multidimensional coupled electron nuclear dynamics involved in the molecular relaxation.