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    Adsorption-induced multiple magnetic phase transitions in monolayer MPX3 (M=V, Mn; X=S, Se, Te)

    Dong Liu, Sike Zeng, Jihai Liao, Yao Yao, and Yu-Jun Zhao*

    • *Contact author: zhaoyj@scut.edu.cn

    Phys. Rev. B 113, 224402 – Published 1 June, 2026

    DOI: https://doi.org/10.1103/lgdz-961s

    Abstract

    Modulating magnetism in two-dimensional (2D) materials is of great importance for the development of spintronics. Although surface adsorption has been demonstrated as an effective approach for tuning electronic and magnetic properties, its application in 2D magnetic materials is still emerging. In this work, we demonstrate that surface adsorption can robustly induce multiple magnetic phase transitions in Néel antiferromagnetic MPX3 monolayers. By selectively adsorbing representative metal (Be, Ca) and highly electronegative nonmetal (O, F) atoms on MPX3 with their corresponding energetically favored configuration, the antiferromagnetic ground state can be transformed into ferromagnetic, altermagnetic, ferrimagnetic, or fully compensated ferrimagnetic states, accompanied by significant nonrelativistic spin splitting. Specifically, adsorption of highly electronegative atoms (such as O and F) breaks the symmetry between opposite spin sublattices, leading to altermagnetism in VPX3, characterized by nonrelativistic spin splitting in the band structure and a symmetry-protected zero net magnetization. In MnPX3, adsorption of electronegative atoms induces a semiconductor-to-half metal transition, and drives an antiferromagnetic-to-ferromagnetic transition. For metal atom adsorbates (e.g., Be, Ca), their favorable configurations break all symmetries connecting opposite spin sublattices, resulting in ferrimagnetic spin splitting in MPX3. When the system remains gapped, appropriate band filling ensures fully compensated magnetization. Our findings provide valuable guidance for designing high-performance spintronic devices based on monolayer MPX3.

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