Electronic Structure and Magnetic Anisotropy of Single-Layer Rare-Earth Oxybromide

The discovery of intrinsic magnetism in two-dimensional (2D) limit has triggered increasing investigations in layered magnetic materials. However, most of the available candidates involves 3d transition metals, while the layered rare-earth magnetic materials are largely unexplored at present. Here, we proposed a series of 2D rare-earth magnetic semiconductors REOBr (RE = Tb, Dy, Ho, Er and Tm) with large magnetic moments and magnetic anisotropy energies using the PBE + U method. Our calculations indicate a half-metallic meta-stable state and a low-energy semi-conducting ground state in these 4f single-layers, which can be characterized by the location of the two-fold degenerate x(x ² - 3y ²) orbital. The dynamical stability of single-layer REOBr is further confirmed using phonon dispersions. The predicted energy gaps ranging from 2.47 to 4.26 eV decrease with the atomic number of the rare-earth element. Meanwhile, very large spin moments and orbital moments up to 6.018 and 2.872 μ_B are found, which seem to be insensitive to the magnetic state. Furthermore, the magnetic anisotropy energies are evaluated and understood by a fourth-order non-uniaxial anisotropy mode. Diverse anisotropy energy landscapes including easy cone, easy plane, and easy axis are found, and an extremely high magnetic anisotropy energy of about 8 meV per RE atom is found in the single-layer DyOBr. Our investigations provide a unique insight into layered rare-earth magnetic materials and suggest the single-layer REOBr as competing candidates for low-dimensional data storage applications.