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 mu(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.