Layer-dependent ferromagnetism in a van der Waals crystal down to the monolayer limit

TLDR: Xu et al. as mentioned in this paper used magneto-optical Kerr effect microscopy to show that monolayer chromium triiodide (CrI3) is an Ising ferromagnet with out-of-plane spin orientation.

Abstract: Magneto-optical Kerr effect microscopy is used to show that monolayer chromium triiodide is an Ising ferromagnet with out-of-plane spin orientation. The question of what happens to the properties of a material when it is thinned down to atomic-scale thickness has for a long time been a largely hypothetical one. In the past decade, new experimental methods have made it possible to isolate and measure a range of two-dimensional structures, enabling many theoretical predictions to be tested. But it has been a particular challenge to observe intrinsic magnetic effects, which could shed light on the longstanding fundamental question of whether intrinsic long-range magnetic order can robustly exist in two dimensions. In this issue of Nature, two groups address this challenge and report ferromagnetism in atomically thin crystals. Xiang Zhang and colleagues measured atomic layers of Cr2Ge2Te6 and observed ferromagnetic ordering with a transition temperature that, unusually, can be controlled using small magnetic fields. Xiaodong Xu and colleagues measured atomic layers of CrI3 and observed ferromagnetic ordering that, remarkably, was suppressed in double layers of CrI3, but restored in triple layers. The two studies demonstrate a platform with which to test fundamental properties of purely two-dimensional magnets. Since the discovery of graphene1, the family of two-dimensional materials has grown, displaying a broad range of electronic properties. Recent additions include semiconductors with spin–valley coupling2, Ising superconductors3,4,5 that can be tuned into a quantum metal6, possible Mott insulators with tunable charge-density waves7, and topological semimetals with edge transport8,9. However, no two-dimensional crystal with intrinsic magnetism has yet been discovered10,11,12,13,14; such a crystal would be useful in many technologies from sensing to data storage15. Theoretically, magnetic order is prohibited in the two-dimensional isotropic Heisenberg model at finite temperatures by the Mermin–Wagner theorem16. Magnetic anisotropy removes this restriction, however, and enables, for instance, the occurrence of two-dimensional Ising ferromagnetism. Here we use magneto-optical Kerr effect microscopy to demonstrate that monolayer chromium triiodide (CrI3) is an Ising ferromagnet with out-of-plane spin orientation. Its Curie temperature of 45 kelvin is only slightly lower than that of the bulk crystal, 61 kelvin, which is consistent with a weak interlayer coupling. Moreover, our studies suggest a layer-dependent magnetic phase, highlighting thickness-dependent physical properties typical of van der Waals crystals17,18,19. Remarkably, bilayer CrI3 displays suppressed magnetization with a metamagnetic effect20, whereas in trilayer CrI3 the interlayer ferromagnetism observed in the bulk crystal is restored. This work creates opportunities for studying magnetism by harnessing the unusual features of atomically thin materials, such as electrical control for realizing magnetoelectronics12, and van der Waals engineering to produce interface phenomena15.