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    Tunable valley polarization and spin splitting in altermagnetic Fe2MoS2X2(X=S,Se,Te) via symmetry engineering

    Quan Shen1, Wenhu Liao1, Hairui Bao1, Degao Xu2, Jianing Tan1,*, Jiansheng Dong1,†, and Gang Ouyang3,‡

    • 1Department of Physics, Jishou University, Jishou 416000, Hunan, China
    • 2School of Physics and Optoelectronic Engineering, Yangtze University, Jingzhou 434023, China
    • 3Key Laboratory of Low-Dimensional Quantum Structures and Quantum Control of Ministry of Education, Key Laboratory for Matter Microstructure and Function of Hunan Province, School of Physics and Electronics, Hunan Normal University, Changsha 410081, China

    • *Contact author: jianingtan@hunnu.edu.cn
    • †Contact author: jsdong@jsu.edu.cn
    • ‡Contact author: gangouy@hunnu.edu.cn

    Phys. Rev. Materials 9, 114404 – Published 10 November, 2025

    DOI: https://doi.org/10.1103/94ll-cldp

    Abstract

    The altermagnetic state combines broken time-reversal symmetry with compensated magnetic order to generate spin-split bands at zero net magnetization and offering promising spintronic functionalities. In this work, we use first-principles calculations to demonstrate deterministic control of valley and spin states in two-dimensional altermagnetic Fe2MoS2X2 (X=S, Se, Te). Monolayer Fe2MoS2Se2 exhibits giant strain tunable valley polarization (58 meV at 4% tensile), while AA1−stacked bilayer Fe2MoS2Se2 show electrically programmable spin splitting (105 meV and 133 meV in X/Y valleys at Ez=0.1V/Å). Spin-flip switching, enabled by magnetic moment reversal and detected via magneto-optical Kerr contrast, emerges as a distinct phenomenon in bilayer Fe2MoS2Se2. These findings establish two-dimensional altermagnetic Fe2MoS2X2 (X=S, Se, Te) as a platform for valleytronics, with design principles applicable to ultra-low-power spintronic devices.

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