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合金化范德华反铁磁体中可调谐的磁激子耦合

Tunable Magneto-Excitonic Coupling in Alloyed van der Waals Antiferromagnet

Maciej Smiertka, Oliwia Janikowska, Katarzyna Olkowska-Pucko, Grzegorz Krasucki, Katarzyna Posmyk, Paulina Peksa, Alessandro Surrente, Dimitar Pashov, Kseniia Mosina, Zdenek Sofer, Mark van Schilfgaarde, Adam Babinski, Maciej R. Molas, Gabriela Komorowska, Esteban Zamora-Amo, Andres Castellanos-Gomez, Federico Mompean, Mar Garcia-Hernandez, Michal Baranowski, Swagata Acharya, Paulina Plochocka

arXiv 2607.14723首次发表:更新:

AI 中文总结

研究在范德华反铁磁体CrSBr中掺入氯对磁光相互作用的影响,结合磁光光谱与GW计算,发现Cl插入使激子波函数局域化,降低磁场诱导的能量重整化,确立成分合金化可调控范德华磁半导体磁光性质耦合。

AI 中文摘要

层状磁半导体中磁序与光生激子(由库仑相互作用束缚的电子 - 空穴对)之间的独特耦合为控制光与物质相互作用提供了有力机制。在范德华反铁磁体CrSBr中,这种耦合异常强烈,在两种共存激子态之间表现明显。本文揭示了通过掺入氯如何重塑CrSBr1 - xClx中的磁光相互作用,结合高达85T的磁光光谱和合金超胞的准粒子自洽GW计算表明,Cl插入使激子波函数逐渐局域化,两种态趋向更类弗伦克尔态,磁场诱导的能量重整化系统降低。该工作将激子特性与磁激子耦合直接联系起来,确立了成分合金化是调控范德华磁半导体磁光性质耦合的有效策略。

英文摘要

The unique coupling between magnetic order and photo-generated excitons, electron-hole pairs bound by Coulomb interaction, in layered magnetic semiconductors offers a powerful mechanism for controlling light-matter interactions. In the van der Waals antiferromagnet CrSBr, this coupling is exceptionally strong and manifests distinctly between two coexisting excitonic states: the localised, Frenkel-like XA exciton and the more delocalised, Wannier-Mott-like XB exciton, providing a unique playground for the optical control of magnetism. Here, we reveal how chlorine incorporation reshapes the magneto-optical interplay in CrSBr1-xClx by simultaneously modifying its electronic structure, excitonic properties, and magnetic interactions. Combining magneto-optical spectroscopy up to 85 T with state-of-the-art quasiparticle self-consistent GW (QSGW) calculations on alloy supercells, we show that Cl insertion progressively localises the excitonic wavefunctions and drives both states toward a more Frenkel-like regime. This evolution is accompanied by a systematic reduction of the magnetic-field-induced energy renormalisation, most prominently for the XB exciton. Our work connects exciton character directly to magneto-excitonic coupling. Furthermore, it establishes compositional alloying as an effective strategy for engineering the coupling between magnetic and optical properties in van der Waals magnetic semiconductors.

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