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Contribution of d-electron to ferroelectricity of type-II multiferroicscauses strong magneto-electric coupling and distinguishes them from theconventional type-I multiferroics. However, their therein polarization is toosmall because the ferroelectricity is merely a derivative from the magneticorder. 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-IImultiferroics. Both ferroelectricity and magnetism arise from the same Vcation, where the filled d-orbital is perpendicular to an a prioriferroelectric polarization and thus poses no hindrance to ferroelectricity,indicating a violation of the usual d0 rule. This makes the combination oflarge polarizations and strong magneto-electric coupling possible. Our findingsnot only add new ferromagnetic-ferroelectric multiferroics, but also point to aunique mechanism to engineer multiferroics.

Two-dimensional ferromagnetic-ferroelectric multiferroics in violation of the d0 rule