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    Exchange-controlled surface linear magnetoelectricity in rutile-type altermagnetic transition metal difluorides

    Jie Wang1, Hefang Cao1, Xinyue Xia1, Yizhang Wu2,3,*, X. S. Wu3,4,*, and Aimei Zhang1,*

    • *Contact author: amzhang2009@hhu.edu.cn

    Phys. Rev. B 113, 184431 – Published 7 May, 2026

    DOI: https://doi.org/10.1103/vh79-rf6t

    Abstract

    Surface magnetoelectric (ME) coupling is conventionally attributed to strong spin-orbit coupling (SOC) or interface-induced polarization and is therefore considered strongly limited in centrosymmetric antiferromagnets. Here we show, theoretically, that rutile-type transition-metal fluorides MF2 (M=V, Mn, Fe, Co, Ni) can exhibit a linear ME response at the (110) surface even in the absence of SOC, enabled by the interplay between bulk magnetic octupolar order and surface symmetry breaking. Our first-principles calculations reveal that ferroically ordered bulk magnetic octupoles in MF2 provide the symmetry prerequisite for a linear surface ME effect. The magnitude of this surface ME coupling is primarily governed by the magnetic exchange energy scale and the extent of interfacial electronic reconstruction. Specifically, in VF2 and CoF2, relatively weak exchange splitting generates pronounced d-orbital surface states near the Fermi level, yielding large displacement-induced surface magnetoelectric coefficients λsurf. In contrast, the strong exchange splitting in MnF2 and FeF2 maintains an insulating surface character and substantially suppresses λsurf. NiF2, featuring nearly degenerate d8 spin configurations (i.e., an electronic configuration with eight electrons occupying the Ni 3d orbitals), further displays nonlinear magnetic reconstruction under small perturbations. These findings establish a general mechanism of “exchange-controlled surface magnetoelectricity” in rutile MF2 compounds, clarify that bulk octupoles act as a symmetry prerequisite rather than the primary determinant of the response amplitude, and render this MF2 family a promising platform for designing tunable, multipole-driven surface ME functionalities.

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