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<p>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 1<i>s</i>&#xa0;→&#xa0;<i>σ</i><sup>*</sup> 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.</p>

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

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年12月29日

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  • Marco Malvestuto,
  • Beatrice Volpato,
  • Elena Babici,
  • Richa Bhardwaj,
  • Antonio Caretta,
  • Simone Laterza,
  • Fulvio Parmigiani,
  • Michele Manfredda,
  • Alberto Simoncig,
  • Marco Zangrando,
  • Alexander Demidovich,
  • Peter Susnjar,
  • Enrico Massimiliano Allaria,
  • Alexander Darius Brynes,
  • David Garzella,
  • Luca Giannessi,
  • Primož Rebernik,
  • Filippo Sottocorona,
  • Dino Novko

摘要

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.