Extreme ultraviolet wave packet interferometry of the autoionizing HeNe dimer

TL;DR

This paper demonstrates femtosecond extreme ultraviolet wave packet interferometry to study ultrafast inter-atomic decay in the HeNe dimer, achieving high temporal and spectral resolution for real-time analysis.

Contribution

It introduces an XUV phase-cycling scheme enabling high-sensitivity interferometry of molecular targets, revealing detailed ICD dynamics.

Findings

Observation of vibronic dephasing and rephasing signatures

Detection of ultrafast decoherence related to ICD

High-resolution molecular absorption spectrum obtained

Abstract

Femtosecond extreme ultraviolet wave packet interferometry (XUV-WPI) was applied to study resonant inter-atomic Coulombic decay (ICD) in the HeNe dimer. The high demands on phase stability and sensitivity for vibronic XUV-WPI of molecular-beam targets are met using an XUV phase-cycling scheme. The detected quantum interferences exhibit vibronic dephasing and rephasing signatures along with an ultrafast decoherence assigned to the ICD process. A Fourier analysis reveals the molecular absorption spectrum with high resolution. The demonstrated experiment shows a promising route for the real-time analysis of ultrafast ICD processes with both high temporal and spectral resolution.