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<p>Excitonics is an emerging field focused on exploiting and manipulating excitons generated through light-matter interactions. Advancing the field into X-ray excitonics requires precise energy and time control of core-exciton resonances, enabling non-linear X-ray phenomena such as element-specific X-ray transient gratings, and advancing material characterization. To achieve these objectives, it is essential to comprehend the role of many-body effects governing core-exciton dynamics. In this work, we address this challenge by combining experiments with an ab initio approach specifically developed to interpret pump-probe excitations. Applied to the prototypical wide-bandgap semiconductor ZnO, first-principles calculations reproduce experimental results and unveil how the density and distribution of photoexcited carriers dynamically tune Coulomb screening, thereby controlling core-exciton binding energies, while Pauli blocking remains negligible. These insights inform a method for dynamically controlling core-exciton resonances at absorption edges, achieving either a uniform spectral blue shift caused by thermalized carrier distributions on picosecond timescales, or distinct blue shifts for individual resonances, driven by time-dependent carrier distributions on femtosecond timescales.</p><p></p>

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Dynamic control of X-ray core-exciton resonances by Coulomb screening in photoexcited semiconductors

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年8月20日

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  • Thomas C. Rossi,
  • Lu Qiao,
  • Conner P. Dykstra,
  • Ronaldo Rodrigues Pela,
  • Richard Gnewkow,
  • Rachel F. Wallick,
  • John H. Burke,
  • Erin Nicholas,
  • Anne Marie March,
  • Gilles Doumy,
  • D. Bruce Buchholz,
  • Christiane Deparis,
  • Jesús Zúñiga-Pérez,
  • Michael Weise,
  • Klaus Ellmer,
  • Mattis Fondell,
  • Claudia Draxl,
  • Renske M. van der Veen

摘要

Excitonics is an emerging field focused on exploiting and manipulating excitons generated through light-matter interactions. Advancing the field into X-ray excitonics requires precise energy and time control of core-exciton resonances, enabling non-linear X-ray phenomena such as element-specific X-ray transient gratings, and advancing material characterization. To achieve these objectives, it is essential to comprehend the role of many-body effects governing core-exciton dynamics. In this work, we address this challenge by combining experiments with an ab initio approach specifically developed to interpret pump-probe excitations. Applied to the prototypical wide-bandgap semiconductor ZnO, first-principles calculations reproduce experimental results and unveil how the density and distribution of photoexcited carriers dynamically tune Coulomb screening, thereby controlling core-exciton binding energies, while Pauli blocking remains negligible. These insights inform a method for dynamically controlling core-exciton resonances at absorption edges, achieving either a uniform spectral blue shift caused by thermalized carrier distributions on picosecond timescales, or distinct blue shifts for individual resonances, driven by time-dependent carrier distributions on femtosecond timescales.