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-spe...
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Nature Portfolio
2025-08-01
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| Series: | Communications Materials |
| Online Access: | https://doi.org/10.1038/s43246-025-00909-w |
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| author | 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 |
| author_facet | 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 |
| author_sort | Thomas C. Rossi |
| collection | DOAJ |
| description | 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. |
| format | Article |
| id | doaj-art-3ee540b2ccff4b5cbde5d425322427ad |
| institution | Kabale University |
| issn | 2662-4443 |
| language | English |
| publishDate | 2025-08-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Communications Materials |
| spelling | doaj-art-3ee540b2ccff4b5cbde5d425322427ad2025-08-24T11:40:51ZengNature PortfolioCommunications Materials2662-44432025-08-01611910.1038/s43246-025-00909-wDynamic control of X-ray core-exciton resonances by Coulomb screening in photoexcited semiconductorsThomas C. Rossi0Lu Qiao1Conner P. Dykstra2Ronaldo Rodrigues Pela3Richard Gnewkow4Rachel F. Wallick5John H. Burke6Erin Nicholas7Anne Marie March8Gilles Doumy9D. Bruce Buchholz10Christiane Deparis11Jesús Zúñiga-Pérez12Michael Weise13Klaus Ellmer14Mattis Fondell15Claudia Draxl16Renske M. van der Veen17Department of Atomic-Scale Dynamics in Light-Energy Conversion (PS-ADLU), Helmholtz-Zentrum Berlin für Materialien und Energie GmbHDepartment of Physics and CSMB, Humboldt-Universität zu BerlinDepartment of Chemistry, University of Illinois Urbana-ChampaignSupercomputing Department, Zuse Institute Berlin (ZIB)Combined X-ray methods at BLiX and BESSY II - SyncLab, Helmholtz-Zentrum Berlin für Materialien und Energie GmbHDepartment of Chemistry, University of Illinois Urbana-ChampaignDepartment of Chemistry, University of Illinois Urbana-ChampaignDepartment of Chemistry, University of Illinois Urbana-ChampaignChemical Sciences and Engineering Division, Argonne National LaboratoryChemical Sciences and Engineering Division, Argonne National LaboratoryDepartment of Materials Science and Engineering, Northwestern UniversityUniversité Côte d’Azur, CNRS, CRHEAUniversité Côte d’Azur, CNRS, CRHEAOptotransmitter-Umweltschutz-Technologie (OUT) e.V.Optotransmitter-Umweltschutz-Technologie (OUT) e.V.Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Institute for Methods and Instrumentation for Synchrotron Radiation ResearchDepartment of Physics and CSMB, Humboldt-Universität zu BerlinDepartment of Atomic-Scale Dynamics in Light-Energy Conversion (PS-ADLU), Helmholtz-Zentrum Berlin für Materialien und Energie GmbHAbstract 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.https://doi.org/10.1038/s43246-025-00909-w |
| spellingShingle | 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 Dynamic control of X-ray core-exciton resonances by Coulomb screening in photoexcited semiconductors Communications Materials |
| title | Dynamic control of X-ray core-exciton resonances by Coulomb screening in photoexcited semiconductors |
| title_full | Dynamic control of X-ray core-exciton resonances by Coulomb screening in photoexcited semiconductors |
| title_fullStr | Dynamic control of X-ray core-exciton resonances by Coulomb screening in photoexcited semiconductors |
| title_full_unstemmed | Dynamic control of X-ray core-exciton resonances by Coulomb screening in photoexcited semiconductors |
| title_short | Dynamic control of X-ray core-exciton resonances by Coulomb screening in photoexcited semiconductors |
| title_sort | dynamic control of x ray core exciton resonances by coulomb screening in photoexcited semiconductors |
| url | https://doi.org/10.1038/s43246-025-00909-w |
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