Vibronic Correlations in Molecular Strong-Field Dynamics

We investigate the ultrafast vibronic dynamics triggered by intense femtosecond infrared pulses in small molecules. Our study is based on numerical simulations performed with 2D model molecules and analyzed in the perspective of the renowned Lochfrass and bond-softening models. We give a new interpretation of the observed nuclear wave packet dynamics with a focus on the phase of the bond oscillations. Our simulations also reveal intricate features in the field-induced nuclear motion that are not accounted for by existing models. Our analyses assign these features to strong dynamical correlations between the active electron and the nuclei, which significantly depend on the carrier envelope phase of the pulse, even for relatively "long" pulses, which should make them experimentally observable.