Ultrafast RIXS of orbital-resolved valence-band reshaping in photoexcited graphite

-edge resonant inelastic x-ray scattering (RIXS), used in the time domain, provides a momentum- and orbital-selective spectroscopic fingerprint of transient valence-band reshaping. Momentum- and orbital-selective measurements along the [Formula: see text] contour disentangle [Formula: see text] and [Formula: see text] contributions and reveal a structured redistribution of spectral weight emerging within ∼70 femtoseconds and evolving on picosecond timescales. Nonequilibrium first-principles RIXS calculations performed within a frozen-lattice approximation show that the earliest response is dominated by electronic correlations and transient screening. At longer delays, the dynamics become strongly momentum dependent: Near [Formula: see text], the signal reflects the decay of the electronic contribution to the renormalized band structure under a hot-phonon bottleneck, whereas at the [Formula: see text]-point van Hove singularity, it reveals a characteristic spectroscopic signature consistent with electron-phonon-driven band red shift and lifetime broadening induced by strongly coupled optical phonons. A three-temperature model constrained by the orbital-resolved tr-RIXS data captures the ensuing energy cascade through a hot-phonon reservoir dominated by the [Formula: see text] and [Formula: see text] modes. These results establish time-domain RIXS as a complementary probe of transient band-structure renormalization and mode-selective energy flow in quantum materials.

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Publication Details

Journal
Science Advances
Published
2026-09-11
DOI
https://doi.org/10.1126/sciadv.aeg6983
Primary Topic
Graphene research and applications
Type
article
Field-Weighted Citation Impact
0.00

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Ultrafast RIXS of orbital-resolved valence-band reshaping in photoexcited graphite

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Ultrafast RIXS of orbital-resolved valence-band reshaping in photoexcited graphite

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article en

Abstract

-edge resonant inelastic x-ray scattering (RIXS), used in the time domain, provides a momentum- and orbital-selective spectroscopic fingerprint of transient valence-band reshaping. Momentum- and orbital-selective measurements along the [Formula: see text] contour disentangle [Formula: see text] and [Formula: see text] contributions and reveal a structured redistribution of spectral weight emerging within ∼70 femtoseconds and evolving on picosecond timescales. Nonequilibrium first-principles RIXS calculations performed within a frozen-lattice approximation show that the earliest response is dominated by electronic correlations and transient screening. At longer delays, the dynamics become strongly momentum dependent: Near [Formula: see text], the signal reflects the decay of the electronic contribution to the renormalized band structure under a hot-phonon bottleneck, whereas at the [Formula: see text]-point van Hove singularity, it reveals a characteristic spectroscopic signature consistent with electron-phonon-driven band red shift and lifetime broadening induced by strongly coupled optical phonons. A three-temperature model constrained by the orbital-resolved tr-RIXS data captures the ensuing energy cascade through a hot-phonon reservoir dominated by the [Formula: see text] and [Formula: see text] modes. These results establish time-domain RIXS as a complementary probe of transient band-structure renormalization and mode-selective energy flow in quantum materials.

Science AdvancesVol. 12(37)
University of Trieste (IT), Elettra-Sincrotrone Trieste S.C.p.A. (IT), Humboldt-Universität zu Berlin (DE), Istituto Officina dei Materiali (IT), Institute of Structure of Matter (IT), Institute of Physics (HR)
Deutsche Forschungsgemeinschaft, Hrvatska Zaklada za Znanost
Affordable and clean energy
Openalex Percentile: Top 24%
Graphene research and applications
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