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Science advances · 2026

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

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Malvestuto Marco, Caretta Antonio, Laterza Simone, Bhardwaj Richa, Volpato Beatrice, Babici Elena, Brondin Carlo Alberto, Manfredda Michele, Simoncig Alberto, Zangrando Marco, Demidovich Alexander, Susnjar Peter, Allaria Enrico Massimiliano, Brynes Alexander Darius, Garzella David, Giannessi Luca, Ribič Primož Rebernik, Sottocorona Filippo, Zamolo Matteo, Hervat Alessandro, Gessini Alessandro, Parmigiani Fulvio, Novko Dino, Richter Elias, Maurer Benedikt, Draxl Claudia

Аннотация

Ultrafast photoexcitation can drive solids far from equilibrium by dynamically renormalizing their electronic structure, yet direct time-domain access to bulk band-structure reshaping with orbital and momentum selectivity has remained limited. Here, we show in photoexcited graphite that femtosecond carbon K-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.

ИП Урсолов Владлен Сергеевич

ИНН 500118482352 · ОГРНИП 314500117700049

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