Charge transfer governed interlayer magnetic coupling and symmetry breaking in a van der Waals magnet

Canyu Hong, Zeyuan Sun (), Zhiyuan Sheng, Shuang Wu, Yi Chen, Ming Tian, Neng Wan, Qixi Mi, Zhongkai Liu, Weibin Chu and Shiwei Wu ()
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Canyu Hong: Fudan University
Zeyuan Sun: Fudan University
Zhiyuan Sheng: Fudan University
Shuang Wu: Fudan University
Yi Chen: ShanghaiTech University
Ming Tian: Southeast University
Neng Wan: Fudan University
Qixi Mi: ShanghaiTech University
Zhongkai Liu: ShanghaiTech University
Weibin Chu: Fudan University
Shiwei Wu: Fudan University

Nature Communications, 2025, vol. 16, issue 1, 1-7

Abstract: Abstract Van der Waals (vdW) magnets provide a rich landscape for innovative spintronic applications at atomic thickness. Among them, chromium sulfide bromide (CrSBr) stands out as a semiconducting antiferromagnet with the potential for magnetoelectric manipulation. However, the detection and electrical control of 2D magnetism in CrSBr are constrained by its centrosymmetric structure and in-plane antiferromagnetism. To address this challenge, we construct heterostructure devices composed of trilayer CrSBr and monolayer graphene, where interfacial charge transfer breaks the inversion symmetry of both magnetic order and crystallographic structure. The inversion symmetry breaking by charge transfer thus allows a full discrimination of the otherwise degenerate magnetic states using optical second harmonic generation, including the charge transfer induced intermediate magnetic states that consist of antiferromagnetic and ferromagnetic vdW interfaces. Furthermore, gate voltage enables the tuning of charge transfer, effectively modulating the interlayer magnetic coupling and magnetic transitions. Our findings deepen the understanding of optospintronic interaction and magnetoelectric manipulation in vdW magnets, paving the way for electrically tunable 2D spintronic devices.

Date: 2025
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DOI: 10.1038/s41467-025-64555-z

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