Mapping Ultrafast Dynamics of Highly Excited D2 by Attosecond XUV Radiation

Using high harmonic generation in a pump-probe geometry, we populate and measure the 2pπu potential in D + 2 . Cold target recoil ion momentum spectroscopy (COLTRIMS) provides the ability to measure full three-dimensional momenta of ion coincidence pairs, enabling full reconstruction of nuclear dynamics. Identification of single ion, ion pair and electron-ion detections confirms the observed state and shows mechanisms through which the nuclear wave packet may be redistributed among other molecular states in a controlled fashion. We quantify the observation via simulation of the time independent Schrödinger equation. Excellent agreement between theory and experiment enables practical implementation of the calculations to further study dynamics. This complete characterization of the potential curve and the dynamics it produces demonstrate a powerful tool poised to study crossings in the 2pπu state, as well as coherent control mechanisms.