Dynamic control of X-ray core-exciton resonances by Coulomb screening in photoexcited semiconductors
Abstract 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.
Authors
- K. Ellmer (ORCID: https://orcid.org/0000-0002-1874-8741)
- Gilles Doumy (ORCID: https://orcid.org/0000-0001-8672-4138)
- Mattis Fondell (ORCID: https://orcid.org/0000-0003-2689-8878)
- John H. Burke (ORCID: https://orcid.org/0000-0001-9853-7292)
- Renske M. van der Veen (ORCID: https://orcid.org/0000-0003-0584-4045)
- Anne Marie March (ORCID: https://orcid.org/0000-0003-2961-1246)
- Jesús Zúñiga-Pérez (ORCID: https://orcid.org/0000-0002-7154-641X)
- Rachel F. Wallick (ORCID: https://orcid.org/0000-0002-7548-4850)
- Thomas Rossi (ORCID: https://orcid.org/0000-0002-7448-8948)
- Claudia Draxl (ORCID: https://orcid.org/0000-0003-3523-6657)
- Erin Nicholas
- Richard Gnewkow (ORCID: https://orcid.org/0000-0002-6524-4909)
- Ronaldo Rodrigues Pelá (ORCID: https://orcid.org/0000-0002-2413-7023)
- Conner Dykstra (ORCID: https://orcid.org/0000-0001-5597-6914)
- Lu Qiao (ORCID: https://orcid.org/0009-0002-0344-1082)
- C. Deparis (ORCID: https://orcid.org/0000-0002-4578-8917)
- D. Bruce Buchholz (ORCID: https://orcid.org/0009-0004-2747-1897)
- Michael J. Weise
Institutions
- Northwestern University (US)
- Argonne National Laboratory (US)
- Centre National de la Recherche Scientifique (FR)
- University of Illinois Urbana-Champaign (US)
- National University of Singapore (SG)
- Nanyang Technological University (SG)
- Zuse Institute Berlin (DE)
- Université Côte d'Azur (FR)
- Helmholtz-Zentrum Berlin für Materialien und Energie (DE)
- Humboldt-Universität zu Berlin (DE)
- Sorbonne Université (FR)
- Institut für Umwelttechnologien (Germany) (DE)
- UMI MajuLab (SG)
- Technische Universität Berlin (DE)
Publication Details
- Journal
- Communications Materials
- Published
- 2025-08-20
- DOI
- https://doi.org/10.1038/s43246-025-00909-w
- Citations
- 1
- Primary Topic
- Electron and X-Ray Spectroscopy Techniques
- Type
- article
- Field-Weighted Citation Impact
- 0.66
Funders
- National Science Foundation
- U.S. Department of Defense
- U.S. Department of Energy
- Alexander von Humboldt-Stiftung
- Northwestern University
- Deutsche Forschungsgemeinschaft
- Office of Science
- Materials Research Science and Engineering Center, Harvard University
- Division of Materials Research
- Division of Electrical, Communications and Cyber Systems
- Basic Energy Sciences
- Argonne National Laboratory