Probing of Core Excitons in Solid NaF with Polarization-Selective Attosecond Time-Resolved Four-Wave Mixing Spectroscopy

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Hauptverfasser: Xiong, Kevin Gulu, Quintero-Bermudez, Rafael, Eggers, Vincent, Laurell, Hugo, Wu, Melody, Leone, Stephen R.
Format: Preprint
Veröffentlicht: 2026
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author Xiong, Kevin Gulu
Quintero-Bermudez, Rafael
Eggers, Vincent
Laurell, Hugo
Wu, Melody
Leone, Stephen R.
author_facet Xiong, Kevin Gulu
Quintero-Bermudez, Rafael
Eggers, Vincent
Laurell, Hugo
Wu, Melody
Leone, Stephen R.
contents Nonlinear Four-wave mixing processes are a powerful technique to unravel ultrafast dynamics in solid-state systems. Here, we employ attosecond four-wave mixing spectroscopy with one extreme ultraviolet (XUV) pump and two independently delayed, noncollinear near-infrared (NIR) probes to resolve the ultrafast decoherence of both dipole-allowed and dipole-forbidden core excitons at the Na+ L2,3 edge in sodium fluoride (NaF). The decoherence times of the core excitons are observed to be much faster than the 8 fs limit of the instrument response time, which is attributed to strong exciton-phonon coupling. Furthermore, polarization control of the NIR probes (Perpendicular and parallel polarizations) reveals that the bright core excitons exhibit s-like orbital angular momentum, while dark core excitons, reached by two-photon excitation, exhibit p-like angular momentum.
format Preprint
id arxiv_https___arxiv_org_abs_2604_06112
institution arXiv
publishDate 2026
record_format arxiv
spellingShingle Probing of Core Excitons in Solid NaF with Polarization-Selective Attosecond Time-Resolved Four-Wave Mixing Spectroscopy
Xiong, Kevin Gulu
Quintero-Bermudez, Rafael
Eggers, Vincent
Laurell, Hugo
Wu, Melody
Leone, Stephen R.
Chemical Physics
Optics
Nonlinear Four-wave mixing processes are a powerful technique to unravel ultrafast dynamics in solid-state systems. Here, we employ attosecond four-wave mixing spectroscopy with one extreme ultraviolet (XUV) pump and two independently delayed, noncollinear near-infrared (NIR) probes to resolve the ultrafast decoherence of both dipole-allowed and dipole-forbidden core excitons at the Na+ L2,3 edge in sodium fluoride (NaF). The decoherence times of the core excitons are observed to be much faster than the 8 fs limit of the instrument response time, which is attributed to strong exciton-phonon coupling. Furthermore, polarization control of the NIR probes (Perpendicular and parallel polarizations) reveals that the bright core excitons exhibit s-like orbital angular momentum, while dark core excitons, reached by two-photon excitation, exhibit p-like angular momentum.
title Probing of Core Excitons in Solid NaF with Polarization-Selective Attosecond Time-Resolved Four-Wave Mixing Spectroscopy
topic Chemical Physics
Optics
url https://arxiv.org/abs/2604.06112