Abstract
CrI3 has raised as an important system to the emergent field of two-dimensional van der Waals magnetic materials. However, it is still unclear why CrI3 which has a ferromagnetic rhombohedral structure in bulk, changed to anti-ferromagnetic monoclinic at thin layers. Here we show that this behaviour is due to the coexistence of both monoclinic and rhombohedral crystal phases followed by three magnetic transitions at TC1 = 61 K, TC2 = 50 K and TC3 = 25 K. Each transition corresponds to a certain fraction of the magnetically ordered volume as well as monoclinic and rhombohedral proportion. The different phases are continuously accessed as a function of the temperature over a broad range of magnitudes. Our findings suggest that the challenge of understanding the magnetic properties of thin layers CrI3 is in general a coexisting structural-phase problem mediated by the volume-wise competition between magnetic phases already present in bulk.
Highlights
CrI3 has raised as an important system to the emergent field of two-dimensional van der Waals magnetic materials
A contrasting case is found in the layered transition metals[7,8,9,10,11] where the presence of heavy halide atoms, like in CrI3, stabilises pronounced anisotropy constants resulting in what appears a homogeneous ferromagnetic phase without any separation[12,13]
Multiple anomalies can be observed in the temperature dependence of the magnetic susceptibility of bulk CrI3 below 61 K16,17,19. Such anomalies imply that a more complex magnetic ordering involving spins not directly aligned with the easy-axis is likely emerging
Summary
CrI3 has raised as an important system to the emergent field of two-dimensional van der Waals magnetic materials It is still unclear why CrI3 which has a ferromagnetic rhombohedral structure in bulk, changed to anti-ferromagnetic monoclinic at thin layers. Multiple anomalies can be observed in the temperature dependence of the magnetic susceptibility of bulk CrI3 below 61 K16,17,19 Such anomalies imply that a more complex magnetic ordering involving spins not directly aligned with the easy-axis is likely emerging. We systematically study the evolution of the magnetic and crystal structures of CrI3 under different temperatures through a synergy of compelling techniques Such approach has resulted being instrumental to identify, characterize and understand the distinct macroscopic ground states observed in this vdW material with competing magnetic and structural phases
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