Signatures of nuclear motion in a model study of ultrafast single-pulse two-photon ionization of diatomic molecules
Phys. Rev. A 114, 022815 – Published 17 August, 2026
DOI: https://doi.org/10.1103/dmyw-c7cq
Abstract
Possible signatures in the photoelectron spectrum of nuclear motion during two-photon single ionization of a diatomic molecule by a single ultraviolet pulse are explored using twelve combinations of model potential curves for initial, near-resonant intermediate, and final cationic electronic states at a range of pulse durations and intensities. From these simulations, we find that a key condition for the photoelectron spectrum to display clear evidence of nuclear motion in the resonant intermediate electronic state during a single pulse is that the dynamics in the intermediate state be significantly different from the vibrational dynamics in both the initial neutral state and the final ionic state of the molecule. Additionally, we present and test a computational approach that explicitly propagates wave packets for nuclear motion on the bound and discretized continuum electronic states.
