Super-moiré spin textures in twisted two-dimensional antiferromagnets

Stacking two-dimensional layered materials offers a platform to engineer electronic and magnetic states. In general, the resulting states-such as moiré magnetism-have a periodicity at the length scale of the moiré unit cell. Here we study magnetic order in twisted double-bilayer chromium triiodide by means of scanning nitrogen-vacancy microscopy. We observe long-range magnetic textures extending beyond the single moiré unit cell, which we dub a super-moiré magnetic state. At small twist angles, the size of the spontaneous magnetic texture increases with twist angle, opposite to the underlying moiré wavelength. The spin-texture size reaches a maximum of about 300 nm in 1.1° twisted devices, an order of magnitude larger than the underlying moiré wavelength, and vanishes at twist angles above 2°. The obtained magnetic field maps suggest the formation of antiferromagnetic Néel-type skyrmions spanning multiple moiré cells. The twist-angle-dependent study, combined with large-scale atomistic Monte Carlo simulations, suggests that the magnetic competition between the Dzyaloshinskii-Moriya interaction, magnetic anisotropy and exchange interactions-which all depend on the relative rotation of the layers-produces the topological textures that emerge in the super-moiré spin order.