Multiple antiferromagnetic phases and magnetic anisotropy in exfoliated CrBr3 multilayers

In twisted two-dimensional (2D) magnets, the stacking dependence of the magnetic exchange interaction can lead to regions of ferromagnetic and antiferromagnetic interlayer order, separated by non-collinear, skyrmion-like spin textures. Recent experimental searches for these textures have focused on CrI 3 , known to exhibit either ferromagnetic or antiferromagnetic interlayer order, depending on layer stacking. However, the very strong uniaxial anisotropy of CrI 3 disfavors smooth non-collinear phases in twisted bilayers. Here, we report the experimental observation of three distinct magnetic phases—one ferromagnetic and two antiferromagnetic—in exfoliated CrBr 3 multilayers, and reveal that the uniaxial anisotropy is significantly smaller than in CrI 3 . These results are obtained by magnetoconductance measurements on CrBr 3 tunnel barriers and Raman spectroscopy, in conjunction with density functional theory calculations, which enable us to identify the stackings responsible for the different interlayer magnetic couplings. The detection of all locally stable magnetic states predicted to exist in CrBr 3 and the excellent agreement found between theory and experiments, provide complete information on the stacking-dependent interlayer exchange energy and establish twisted bilayer CrBr 3 as an ideal system to deterministically create non-collinear magnetic phases. Van der Waals materials often exhibit different metastable structures, with the constituent layers shifted by small, atomic scale distances. If the material is magnetic, the resulting different layer stackings can cause drastic changes in magnetic ordering. Here, Yao et al. observe all three locally stable magnetic orderings predicted to occur in CrBr 3 multilayers, two antiferromagnetic and one ferromagnetic.