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

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.