Imaging the state-to-state charge-transfer dynamics between the spin-orbit excited Ar+(2P1/2) ion and N2

Abstract

Ar++N2 → Ar+N2+ has served as a paradigm for charge-transfer dynamics studies during the last several decades. Despite significant experimental and theoretical efforts on this model system, state-resolved experimental investigations on the microscopic charge-transfer mechanism between the spin-orbit excited Ar+(2P1/2) ion and N2 have been rare. Here, we measure the first quantum state-to-state differential cross sections for Ar++N2 → Ar+N2+ with the Ar+ ion prepared exclusively in the spin-orbit excited state 2P1/2 on a crossed-beam setup with three-dimensional velocity-map imaging. Trajectory surface-hopping calculations qualitatively reproduce the vibrationally dependent rotational and angular distributions of the N2+ product. Both the scattering images and theoretical calculations show that the charge-transfer dynamics of the spin-orbit excited Ar+(2P1/2) ion differs significantly from that of the spin-orbit ground Ar+(2P3/2) when colliding with N2. Such state-to-state information makes quantitative understanding of this benchmark charge-transfer reaction within reach.