Vibronic Correlations in Molecular Strong-Field Dynamics

Abstract

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.

Virtual Special Issue on Attosecond Chemistry

“…Pandey et al present a theoretical study of the coupled electron–nuclear dynamics in the H 2 + molecular ion under the influence of an intense laser field, using both quantum and classical dynamical methods to analyze the validity of simpler classical methods for the description of strong-field phenomena involving both electronic and nuclear motions . Labeye et al have investigated the ultrafast vibronic dynamics triggered by intense femtosecond infrared pulses in small molecules . They provide a new interpretation of the observed nuclear wave packet dynamics and reveal intricate features in the field-induced nuclear motion that are not accounted for by existing models.…”