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.