Coexisting ferromagnetic–antiferromagnetic state in twisted bilayer CrI3

Moiré engineering1-3 of van der Waals magnetic materials4-9 can yield new magnetic ground states via competing interactions in moiré superlattices10-13. Theory predicts a suite of interesting phenomena, including multiflavour magnetic states10, non-collinear magnetic states10-13, moiré magnon bands and magnon networks14 in twisted bilayer magnetic crystals, but so far such non-trivial magnetic ground states have not emerged experimentally. Here, by utilizing the stacking-dependent interlayer exchange interactions in two-dimensional magnetic materials15-18, we demonstrate a coexisting ferromagnetic (FM) and antiferromagnetic (AF) ground state in small-twist-angle CrI3 bilayers. The FM-AF state transitions to a collinear FM ground state above a critical twist angle of about 3°. The coexisting FM and AF domains result from a competition between the interlayer AF coupling, which emerges in the monoclinic stacking regions of the moiré superlattice, and the energy cost for forming FM-AF domain walls. Our observations are consistent with the emergence of a non-collinear magnetic ground state with FM and AF domains on the moiré length scale10-13. We further employ the doping dependence of the interlayer AF interaction to control the FM-AF state by electrically gating a bilayer sample. These experiments highlight the potential to create complex magnetic ground states in twisted bilayer magnetic crystals, and may find application in future gate-voltage-controllable high-density magnetic memory storage.