Coexistence of Magnetic Orders in Two-Dimensional Magnet CrI₃

The magnetic properties in two-dimensional van der Waals materials depend sensitively on structure. CrI₃, as an example, has been recently demonstrated to exhibit distinct magnetic properties depending on the layer thickness and stacking order. Bulk CrI₃ is ferromagnetic (FM) with a Curie temperature of 61 K and a rhombohedral layer stacking, whereas few-layer CrI₃ has a layered antiferromagnetic (AFM) phase with a lower ordering temperature of 45 K and a monoclinic stacking. In this work, we use cryogenic magnetic force microscopy to investigate CrI₃ flakes in the intermediate thickness range (25–200 nm) and find that the two types of magnetic orders, hence the stacking orders, can coexist in the same flake with a layer of ∼13 nm at each surface being in the layered AFM phase similar to few-layer CrI₃ and the rest in the bulk FM phase. The switching of the bulk moment proceeds through a remnant state with nearly compensated magnetic moment along the c-axis, indicating formation of c-axis domains allowed by a weak interlayer coupling strength in the rhombohedral phase. Our results provide a comprehensive picture on the magnetism in CrI₃ and point to the possibility of engineering magnetic heterostructures within the same material.