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

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Autori principali: Yanez-Pagans, S., Alarcon, M. A., Greene, C. H., Sandhu, A.
Natura: Preprint
Pubblicazione: 2025
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author Yanez-Pagans, S.
Alarcon, M. A.
Greene, C. H.
Sandhu, A.
author_facet Yanez-Pagans, S.
Alarcon, M. A.
Greene, C. H.
Sandhu, A.
contents Radiative nonlinear four-wave mixing can monitor the evolution of electronic wave packets, providing access to lifetimes and quantifies the light induced couplings between excited states. We report the observation of quantum beats in an autoionizing electronic wavepacket 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, that quantitatively reproduces both the wavepacket dynamics and the static spectrum. This work combines a versatile, background-free experimental scheme with a tractable model, establishing a powerful approach for the metrology and control of complex, correlated electronic states.
format Preprint
id arxiv_https___arxiv_org_abs_2507_03845
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Probing coherent electronic superpositions of singly- and doubly-excited states of krypton with attosecond four-wave mixing spectroscopy
Yanez-Pagans, S.
Alarcon, M. A.
Greene, C. H.
Sandhu, A.
Atomic Physics
Optics
Quantum Physics
Radiative nonlinear four-wave mixing can monitor the evolution of electronic wave packets, providing access to lifetimes and quantifies the light induced couplings between excited states. We report the observation of quantum beats in an autoionizing electronic wavepacket 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, that quantitatively reproduces both the wavepacket dynamics and the static spectrum. This work combines a versatile, background-free experimental scheme with a tractable model, establishing a powerful approach for the metrology and control of complex, correlated electronic states.
title Probing coherent electronic superpositions of singly- and doubly-excited states of krypton with attosecond four-wave mixing spectroscopy
topic Atomic Physics
Optics
Quantum Physics
url https://arxiv.org/abs/2507.03845