Extreme Ultraviolet Wave Packet Interferometry of the Autoionizing HeNe Dimer

J Phys Chem Lett. 2022 Sep 15;13(36):8470-8476. doi: 10.1021/acs.jpclett.2c01619. Epub 2022 Sep 2.

Abstract

Femtosecond extreme ultraviolet wave packet interferometry (XUV-WPI) was applied to study resonant interatomic 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 high spectral resolution.