Time-Resolved Ultrafast Interatomic Coulombic Decay in Superexcited Sodium-Doped Helium Nanodroplets

J Phys Chem Lett. 2022 May 26;13(20):4470-4478. doi: 10.1021/acs.jpclett.2c00645. Epub 2022 May 13.

Abstract

The autoionization dynamics of superexcited superfluid He nanodroplets doped with Na atoms is studied by extreme-ultraviolet (XUV) time-resolved electron spectroscopy. Following excitation into the higher-lying droplet absorption band, the droplet relaxes into the lowest metastable atomic 1s2s 1,3S states from which interatomic Coulombic decay (ICD) takes place either between two excited He atoms or between an excited He atom and a Na atom attached to the droplet surface. Four main ICD channels are identified, and their decay times are determined by varying the delay between the XUV pulse and a UV pulse that ionizes the initial excited state and thereby quenches ICD. The decay times for the different channels all fall in the range of ∼1 ps, indicating that the ICD dynamics are mainly determined by the droplet environment. A periodic modulation of the transient ICD signals is tentatively attributed to the oscillation of the bubble forming around the localized He excitation.