Two-center Interferences in Photoionization of Dissociating H$_2^+$ Molecule

TL;DR

This paper investigates two-center interference effects in the photoionization of a dissociating H$_2^+$ molecule using ultrashort VUV laser pulses, combining numerical simulations and an analytical model to analyze interference oscillations and nuclear wavepacket dynamics.

Contribution

It introduces a combined numerical and analytical approach to study interference effects in molecular ionization and demonstrates how to extract nuclear wavepacket information from interference patterns.

Findings

Interference oscillations depend on the time delay between pulses.

Resonance with the $\sigma_g - \sigma_u$ transition is crucial.

Nuclear wavepacket spreading reduces oscillation amplitudes.

Abstract

We analyze two-center interference effects in the yields of ionization of a dissociating hydrogen molecular ion by an ultrashort VUV laser pulse. To this end, we performed numerical simulations of the time-dependent Schr\"odinger equation for a H$_2^+$ model ion interacting with two time-delayed laser pulses. The scenario considered corresponds to a pump-probe scheme, in which the first (pump) pulse excites the molecular ion to the first excited dissociative state and the second (probe) pulse ionizes the electron as the ion dissociates. The results of our numerical simulations for the ionization yield as a function of the time delay between the two pulses exhibit characteristic oscillations due to interferences between the partial electron waves emerging from the two protons in the dissociating hydrogen molecular ion. We show that the photon energy of the pump pulse should be in resonance with the $\sigma_g - \sigma_u$ transition and the pump pulse duration should not exceed 5 fs in order to generate a well confined nuclear wavepacket. The spreading of the nuclear wavepacket during the dissociation is found to cause a decrease of the amplitudes of the oscillations as the time delay increases. We develop an analytical model to fit the oscillations and show how dynamic information about the nuclear wavepacket, namely velocity, mean internuclear distance and spreading, can be retrieved from the oscillations. The predictions of the analytical model are tested well against the results of our numerical simulations.