Revealing correlated electronic and nuclear dynamics in molecules with energy-resolved population imaging

Abstract

We explore a method, named energy-resolved population imaging (EPI), to analyze on an equal footing the temporary electronic transition and nuclear motion during laser-molecular interaction. By using EPI we have intuitively demonstrated the population transfer in vibrational ${{\text{H}}_{2}}^{+}$ exposed to extreme ultraviolet pulses, revealing the energy-sharing rule for the correlated electron and nuclei. We further show that EPI can be extended to uncover the origins of the distinct energy-sharing mechanisms in multiphoton and tunneling regimes. The present study has clarified a long-standing issue about the dissociative ionization of ${{\text{H}}_{2}}^{+}$ and paves the way to identify instantaneous molecular dynamics in strong fields.