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Multiferroics are rare in nature due to the mutual exclusive origins of magnetism and ferroelectricity. The simultaneous coexistence of robust magnetism/ferroelectricity and strong magnetoelectric coupling in single multiferroics is hitherto unreported, which may also be attributed to their potential conflictions. In this paper, we show the first-principles evidence of such desired coexistence in ultrathin-layer CuCrS2 and CuCrSe2. The vertical ferroelectricity is neither induced by an empty d shell nor spin-driven, giving rise to an alternative possibility of resolving those intrinsic exclusions and contradictions. Compared with their bulk phases, the ferromagnetism in the thin-layer structures (two-six layers) can be greatly stabilized due to the enhanced carrier density and orbital shifting by vertical polarization, and the Curie temperatures of both ferromagnetism and ferroelectricity can be above room temperature. Moreover, a considerable net magnetization can be reversed upon ferroelectric switching, where the change in spin-resolved band structure also renders efficient 'magnetic reading + electrical writing'. The thickness-different layers may even exhibit diversified types of magnetoelectric coupling, which both enriches the physics of multiferroics and facilitates their practical applications.
Zhong et al. (Thu,) studied this question.