Moiré Skyrmions and Chiral Magnetic Phases in Twisted CrX3 (X = I, Br, and Cl) Bilayers

We present a comprehensive theory of the magnetic phases in twisted bilayer chromium trihalides through a combination of first-principles calculations and atomistic simulations. We show that the stacking-dependent interlayer exchange leads to an effective moiré field that is mostly ferromagnetic with antiferromagnetic patches. A wide range of noncollinear magnetic phases can be stabilized as a function of the twist angle and Dzyaloshinskii–Moriya interaction as a result of the competing interlayer antiferromagnetic coupling and the energy cost for forming domain walls. In particular, we demonstrate that for small twist angles various skyrmion crystal phases can be stabilized in both CrI3 and CrBr3. Our results provide an interpretation for the recent observation of noncollinear magnetic phases in twisted bilayer CrI3 and demonstrate the possibility of engineering further nontrivial magnetic ground states in twisted bilayer chromium trihalides.