Abstract
The recent discovery of two-dimensional (2D) magnets, with a number of interesting magnetic properties, has drawn much interest due to their potential for future 2D spintronic device applications. CrI3, a van der Waals magnet, exhibits two-dimensional ferromagnetism even in monolayer form, stabilized by strong magnetic anisotropy. Its interlayer magnetic ordering is coupled to structural layer stacking, implying that the charge density distribution mediating van der Waals interactions plays a key role in the magnetic interaction between the layers. Using polarization-dependent x-ray spectroscopy, we investigated the response of the electronic environment around Cr and I sites to structural changes of layer stacking order. The highly anisotropic nature of the Cr local environment is significantly enhanced and is accompanied by changes in the valence band, in the rhombohedral phase. Magnetic spectroscopy measurements reveal a sizable iodine orbital moment, indicating the iodine contribution to magnetic anisotropy. Our results uncover an important role for the extended nature of anisotropic Cr orbital states in dictating interlayer magnetic interactions and the iodine contribution to magnetic anisotropy.
