Contribution of d-electron to ferroelectricity of type-II multiferroics causes strong magneto-electric coupling and distinguishes them from the conventional type-I multiferroics. However, their therein polarization is too small because the ferroelectricity is merely a derivative from the magnetic order. Here we report a new class of multiferroic materials, monolayer VOX2 (X = Cl, Br, and I), which combine the advantages of type-I and type-II multiferroics. Both ferroelectricity and magnetism arise from the same V cation, where the filled d-orbital is perpendicular to an a priori ferroelectric polarization and thus poses no hindrance to ferroelectricity, indicating a violation of the usual d0 rule. This makes the combination of large polarizations and strong magneto-electric coupling possible. Our findings not only add new ferromagnetic-ferroelectric multiferroics, but also point to a unique mechanism to engineer multiferroics.
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