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    Probing of core excitons in solid NaF with polarization-selective attosecond time-resolved four-wave mixing spectroscopy

    Kevin Gulu Xiong1,*, Rafael Quintero-Bermudez1,2,3, Vincent Eggers1,†, Hugo Laurell1,3,4,5, Melody Wu3, and Stephen R. Leone1,2,3,‡

    • *Contact author: gkxiong@berkeley.edu
    • †Present address: Department of Physics and Regensburg Center for Ultrafast Nanoscopy (RUN), University of Regensburg, 93040 Regensburg, Germany.
    • ‡Contact author: srl@berkeley.edu

    Phys. Rev. B 114, 105120 – Published 14 August, 2026

    DOI: https://doi.org/10.1103/dn88-cg3j

    Abstract

    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 orbital angular momentum.

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