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Two-dimensional van der Waals Janus materials and their heterostructuresoffer fertile platforms for designing fascinating functionalities. Here, bymeans of systematic first-principles studies on van der Waals Janus monolayerCr-based dichalcogenide halides CrYX (Y=S, Se, Te; X=Cl, Br, I), we find thatCrSX (X=Cl, Br, I) are the very desirable high TC ferromagnetic semiconductorswith an out-of-plane magnetization. Excitingly, by the benefit of the largemagnetic moments on ligand S2- anions, the sought-after large-gap quantumanomalous Hall effect and sizable valley splitting can be achieved through themagnetic proximity effect in van der Waals heterostructures CrSBr/Bi2Se3/CrSBrand MoTe2/CrSBr, respectively. Additionally, we show that largeDzyaloshinskii-Moriya interactions give rise to skyrmion states in CrTeX (X=Cl,Br, I) under external magnetic fields. Our work reveals that two-dimensionalJanus magnet Cr-based dichalcogenide halides have appealingmultifunctionalities in the applications of topological electronic andvalleytronic devices.

Multifunctional Two-dimensional van der Waals Janus Magnet Cr-based Dichalcogenide Halides