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Owing to unique fundamental physics and device applications, twisted moiré physics in two-dimensional (2D) van der Waals (vdW) layered magnetic materials has recently received particular attention. We investigate magnetic vdW Fe 3 GeTe 2  (FGT)/CrGeTe 3  (CGT) moiré heterobilayers with twist angles of 11° and 30° from first-principles. We show that the moiré heterobilayer is a ferromagnetic metal with an  n -type CGT layer due to the dominant spin-majority electron transfer from the FGT layer to the CGT layer, regardless of various stacked structures. The spin-majority hybridized bands between Cr and Fe bands crossing the Fermi level are found regardless of stacking. The band alignment of the CGT layer depends on the effective potential difference at the interface. We show that an external electric field perpendicular to the in-plane direction modulates the interface dipole and band edges. Our study reveals a deeper understanding of the effects of stacking, spin alignment, spin transfer, and electrostatic gating on the 2D vdW magnetic metal/semiconductor heterostructure interface.

Hybridized bands and stacking-dependent band edges in ferromagnetic Fe3GeTe2/CrGeTe3 moiré heterobilayer