De- and Recoherence of Charge Migration in IonizedIodoacetylene

During charge migration electrons flow rapidly from one site of a molecule to another, perhaps inducing subsequent processes (e.g., selective breaking of chemical bonds). The first joint experimental and theoretical preparation and measurement of the initial state and subsequent quantum dynamics simulation of charge migration for fixed nuclei was demonstrated recently for oriented, ionized iodoacetylene. Here we present new quantum dynamics simulations for the same system with moving nuclei. They reveal the decisive role of the nuclei, i.e. they switch charge migration off (“decoherence”) and on (“recoherence”). This is a new finding in attosecond-to-femtosecond chemistry and physics which opens new prospects for laser control over electronic dynamics via nuclear motions.