Time-resolved resonant inelastic X-ray scattering (tr-RIXS) is a powerful technique for probing quasiparticle interactions in quantum materials under nonequilibrium conditions. Here, we implement tr-RIXS at the carbon K-edge to investigate the ultrafast dynamics of core excitons coupled to vibrational modes in graphite. Using femtosecond X-ray pulses from a free-electron laser, we monitor the temporal evolution of vibronically dressed excitons and their interaction with symmetry-selective optical phonons. By tuning the incident photon energy across the 1s → σ* resonance and analyzing the integrated inelastic sideband intensity, we reveal a detuning-controlled crossover between two complementary dynamical regimes. Phenomenological modeling and first-principles calculations reproduce both the magnitude and detuning dependence of the spectral-weight changes. In this work, enabled by the unique capabilities of X-ray free-electron lasers, we demonstrate how tr-RIXS can access coupled electronic and lattice dynamics with elemental and symmetry specificity, opening new routes to control vibronic interactions in light-element and low-dimensional quantum materials.

Ultrafast dynamics of vibronically dressed core excitons in graphite: a femtosecond RIXS perspective

Marco Malvestuto;Fulvio Parmigiani;Marco Zangrando;
2025

Abstract

Time-resolved resonant inelastic X-ray scattering (tr-RIXS) is a powerful technique for probing quasiparticle interactions in quantum materials under nonequilibrium conditions. Here, we implement tr-RIXS at the carbon K-edge to investigate the ultrafast dynamics of core excitons coupled to vibrational modes in graphite. Using femtosecond X-ray pulses from a free-electron laser, we monitor the temporal evolution of vibronically dressed excitons and their interaction with symmetry-selective optical phonons. By tuning the incident photon energy across the 1s → σ* resonance and analyzing the integrated inelastic sideband intensity, we reveal a detuning-controlled crossover between two complementary dynamical regimes. Phenomenological modeling and first-principles calculations reproduce both the magnitude and detuning dependence of the spectral-weight changes. In this work, enabled by the unique capabilities of X-ray free-electron lasers, we demonstrate how tr-RIXS can access coupled electronic and lattice dynamics with elemental and symmetry specificity, opening new routes to control vibronic interactions in light-element and low-dimensional quantum materials.
2025
Istituto Officina dei Materiali - IOM -
rixs, fel, laser, diagnostica
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Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/20.500.14243/583026
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