Long Lived Electronic Coherences in Molecular Wave Packets Probed with Pulse Shape Spectroscopy

Abstract

We explore long lived electronic coherences in molecules using shaped ultrafast laser pulses to launch and probe entangled nuclear-electronic wave packets. We find that under certain conditions, the electronic phase remains well defined despite vibrational motion along many degrees of freedom. The experiments are interpreted with the help of electronic structure calculations which corroborate our interpretation of the measurement