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    Magnetoelectric hysteresis in van der Waals antiferromagnetic insulator MnPS3 single crystals

    Yongsen Tang1,*, Juan Wang1, Hanyan Wang2, Bing Yu3, Yakui Weng1, Shuang Zhou1, Hao Chen1, Hongguang Zhang1,†, and Xing'ao Li1,‡

    • *Contact author: tangys@njupt.edu.cn
    • †Contact author: zhanghg@njupt.edu.cn
    • ‡Contact author: lxahbmy@126.com

    Phys. Rev. Materials 10, 094404 – Published 14 September, 2026

    DOI: https://doi.org/10.1103/2j2d-vldd

    Abstract

    We report a systematic investigation of the structural, magnetic, and magnetoelectric properties of single-crystalline MnPS3, a van der Waals honeycomb antiferromagnetic insulator. While isostructural to MnPSe3, MnPS3 exhibits distinct magnetic behavior characterized by a Néel temperature of TN∼78 K and a magnetic point group 2′/m with moments oriented predominantly along the c axis. Thermodynamic analysis via specific heat reveals a significant magnetic entropy release extending well above TN, indicative of robust two-dimensional short-range correlations and a two-/three-dimensional magnetic crossover. Crucially, we observe a magnetic-field-induced electric polarization ΔPz when a magnetic field is applied perpendicular to the z direction. The ΔPz(H) response exhibits a pronounced and unconventional hysteretic behavior, which we attribute to the interplay between the symmetry-allowed linear ME effect and weak interlayer vdW interactions that govern magnetic domain dynamics. These findings provide fundamental insights into the symmetry-driven magnetoelectric coupling in low-dimensional systems and position MnPS3 as a versatile platform for tunable spintronic and quantum functional devices.

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