Magnetism and stability of all primitive stacking patterns in bilayer chromium trihalides

Chromium trihalides, CrX3 (with X = Cl, Br, I), are a family of layered magnetic materials that can be easily exfoliated to provide ferromagnetic monolayers. When two layers are stacked together to form a bilayer the interlayer exchange coupling can be either ferromagnetic or antiferromagnetic depending on the stacking sequence. Here we combine crystallographic arguments based on the close-packing condition with first-principles simulations to enumerate all possible stacking patterns in CrX3 bilayers that preserve the spatial periodicity of each layer. We recover all configurations observed in bulk crystals and disclose stacking sequences with no bulk counterpart where the two layers have opposite chirality. Stacking sequences are ranked according to their relative stability and a preferential interlayer magnetic ordering is assigned to each of them. Simulations provide a consistent picture to frame all current experimental observations on bulk and exfoliated CrX3 crystals, with interesting implications for future measurements, including synthetic bilayers with non-standard stacking patterns.

Automated summary

Chromium trihalides in bilayer form can exhibit either ferromagnetic or antiferromagnetic interlayer exchange coupling depending on the stacking sequence. Crystallographic arguments and first-principles simulations were used to enumerate all possible stacking patterns, ranking them based on relative stability. The simulations provide a consistent framework for understanding experimental observations on bulk and exfoliated CrX3 crystals, with implications for future measurements.