Large exciton binding energy in a bulk van der Waals magnet from quasi-1D electronic localization

Abstract Excitons, bound electron-hole pairs, influence the optical properties in strongly interacting solid-state systems and are typically most stable and pronounced in monolayer materials. Bulk systems with large exciton binding energies, on the other hand, are rare and the mechanisms driving the...

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Main Authors: Shane Smolenski, Ming Wen, Qiuyang Li, Eoghan Downey, Adam Alfrey, Wenhao Liu, Aswin L. N. Kondusamy, Aaron Bostwick, Chris Jozwiak, Eli Rotenberg, Liuyan Zhao, Hui Deng, Bing Lv, Dominika Zgid, Emanuel Gull, Na Hyun Jo
Format: Article
Language:English
Published: Nature Portfolio 2025-01-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-025-56457-x
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author Shane Smolenski
Ming Wen
Qiuyang Li
Eoghan Downey
Adam Alfrey
Wenhao Liu
Aswin L. N. Kondusamy
Aaron Bostwick
Chris Jozwiak
Eli Rotenberg
Liuyan Zhao
Hui Deng
Bing Lv
Dominika Zgid
Emanuel Gull
Na Hyun Jo
author_facet Shane Smolenski
Ming Wen
Qiuyang Li
Eoghan Downey
Adam Alfrey
Wenhao Liu
Aswin L. N. Kondusamy
Aaron Bostwick
Chris Jozwiak
Eli Rotenberg
Liuyan Zhao
Hui Deng
Bing Lv
Dominika Zgid
Emanuel Gull
Na Hyun Jo
author_sort Shane Smolenski
collection DOAJ
description Abstract Excitons, bound electron-hole pairs, influence the optical properties in strongly interacting solid-state systems and are typically most stable and pronounced in monolayer materials. Bulk systems with large exciton binding energies, on the other hand, are rare and the mechanisms driving their stability are still relatively unexplored. Here, we report an exceptionally large exciton binding energy in single crystals of the bulk van der Waals antiferromagnet CrSBr. Utilizing state-of-the-art angle-resolved photoemission spectroscopy and self-consistent ab-initio GW calculations, we present direct spectroscopic evidence supporting electronic localization and weak dielectric screening as mechanisms contributing to the amplified exciton binding energy. Furthermore, we report that surface doping enables broad tunability of the band gap offering promise for engineering of the optical and electronic properties. Our results indicate that CrSBr is a promising material for the study of the role of anisotropy in strongly interacting bulk systems and for the development of exciton-based optoelectronics.
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issn 2041-1723
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publishDate 2025-01-01
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spelling doaj-art-6a034e31d677420c96b1c57d90cd42b22025-02-02T12:33:21ZengNature PortfolioNature Communications2041-17232025-01-011611810.1038/s41467-025-56457-xLarge exciton binding energy in a bulk van der Waals magnet from quasi-1D electronic localizationShane Smolenski0Ming Wen1Qiuyang Li2Eoghan Downey3Adam Alfrey4Wenhao Liu5Aswin L. N. Kondusamy6Aaron Bostwick7Chris Jozwiak8Eli Rotenberg9Liuyan Zhao10Hui Deng11Bing Lv12Dominika Zgid13Emanuel Gull14Na Hyun Jo15Department of Physics, University of MichiganDepartment of Chemistry, University of MichiganDepartment of Physics, University of MichiganDepartment of Physics, University of MichiganApplied Physics Program, University of MichiganDepartment of Physics, The University of Texas at DallasDepartment of Materials Science and Engineering, The University of Texas at DallasAdvanced Light Source, Lawrence Berkeley National LaboratoryAdvanced Light Source, Lawrence Berkeley National LaboratoryAdvanced Light Source, Lawrence Berkeley National LaboratoryDepartment of Physics, University of MichiganDepartment of Physics, University of MichiganDepartment of Physics, The University of Texas at DallasDepartment of Physics, University of MichiganDepartment of Physics, University of MichiganDepartment of Physics, University of MichiganAbstract Excitons, bound electron-hole pairs, influence the optical properties in strongly interacting solid-state systems and are typically most stable and pronounced in monolayer materials. Bulk systems with large exciton binding energies, on the other hand, are rare and the mechanisms driving their stability are still relatively unexplored. Here, we report an exceptionally large exciton binding energy in single crystals of the bulk van der Waals antiferromagnet CrSBr. Utilizing state-of-the-art angle-resolved photoemission spectroscopy and self-consistent ab-initio GW calculations, we present direct spectroscopic evidence supporting electronic localization and weak dielectric screening as mechanisms contributing to the amplified exciton binding energy. Furthermore, we report that surface doping enables broad tunability of the band gap offering promise for engineering of the optical and electronic properties. Our results indicate that CrSBr is a promising material for the study of the role of anisotropy in strongly interacting bulk systems and for the development of exciton-based optoelectronics.https://doi.org/10.1038/s41467-025-56457-x
spellingShingle Shane Smolenski
Ming Wen
Qiuyang Li
Eoghan Downey
Adam Alfrey
Wenhao Liu
Aswin L. N. Kondusamy
Aaron Bostwick
Chris Jozwiak
Eli Rotenberg
Liuyan Zhao
Hui Deng
Bing Lv
Dominika Zgid
Emanuel Gull
Na Hyun Jo
Large exciton binding energy in a bulk van der Waals magnet from quasi-1D electronic localization
Nature Communications
title Large exciton binding energy in a bulk van der Waals magnet from quasi-1D electronic localization
title_full Large exciton binding energy in a bulk van der Waals magnet from quasi-1D electronic localization
title_fullStr Large exciton binding energy in a bulk van der Waals magnet from quasi-1D electronic localization
title_full_unstemmed Large exciton binding energy in a bulk van der Waals magnet from quasi-1D electronic localization
title_short Large exciton binding energy in a bulk van der Waals magnet from quasi-1D electronic localization
title_sort large exciton binding energy in a bulk van der waals magnet from quasi 1d electronic localization
url https://doi.org/10.1038/s41467-025-56457-x
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