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Limited calculations show that monolayer (ML) chromium dichalcogenide (CrS2) has a direct bandgap and valley polarization but with a smaller bandgap than ML MoS2 and with distinct piezoelectric and ferromagnetic properties. It is highly desirable to determine an appropriate metal contact for novel two‐dimensional (2D) CrS2‐based devices. By using density functional theory (DFT), the interface between...