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

TL;DR

This paper demonstrates the use of shaped ultrafast laser pulses to observe long-lived electronic coherences in molecules, revealing phase stability despite vibrational dynamics, supported by electronic structure calculations.

Contribution

It introduces pulse shape spectroscopy as a method to probe and understand long-lived electronic coherences in molecular wave packets.

Findings

Electronic phase remains well defined despite vibrational motion.

Shaped ultrafast laser pulses can effectively probe electronic coherences.

Electronic structure calculations support experimental observations.

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 measurements