Work

Probing coherent electronic superpositions of singly and doubly excited states of krypton with extreme-ultraviolet four-wave-mixing spectroscopy

Year: 2025

Type: article

Abstract: Radiative nonlinear four-wave mixing can monitor the evolution of electronic wave packets, providing access to lifetimes and quantifying the light-induced couplings between excited states. We report the observation of quantum beats in an autoionizing electronic wave packet in krypton, probed using this technique. Analysis of the signal reveals that these beats originate from the contribution of previously unassigned, doubly excited states interacting with singly excited ones. We introduce a minimal theoretical model, based on multichannel quantum-defect theory, which quantitatively reproduces both the wave-packet dynamics and the static spectrum. This work combines a versatile, noncommensurate XUV-IR-based experimental scheme with a tractable model, establishing a powerful approach for the metrology and control of complex, correlated electronic states.

Source: Physical Review A

DOI: 10.1103/5sld-ds77

Authors: S. Yanez-Pagans, M. A. Alarcón, C. H. Greene, A. Sandhu

Institutions: University of Arizona, Purdue University West Lafayette, Arizona State University

Language: English

Topic: Laser-Matter Interactions and Applications

Subfield: Atomic and Molecular Physics, and Optics

Field: Physics and Astronomy

Domain: Physical Sciences

Open Access status: green

Funder: U.S. Department of Energy

Awards: LIGHT-INDUCED MODIFICATION OF ELECTRONIC INTERACTIONS AND ELECTRON-NUCLEAR COUPLINGS, PHYSICS OF CORRELATED SYSTEMS