CrO<sub>2</sub> monolayer: a two-dimensional ferromagnet with high Curie temperature and half-metallicity

Abstract

Owing to the complete spin-polarization of electronic states near Fermi energy, half-metallic ferromagnets, especially two-dimensional half-metallic ferromagnets, have garnered significant attention in the field of spintronics. However, the practical application of these materials is greatly hindered by their low Curie temperatures. Therefore, the exploration of high Curie temperature half-metallic ferromagnets poses a necessary and challenging task. In this study, we predict a two-dimensional transition metal oxide, CrO<sub>2</sub> monolayer, and employed first-principles calculations to investigate the crystal structure, electronic properties, magnetic ground state, and ferromagnetic phase transition. The calculations on phonon spectrum, elastic constant, and molecular dynamics simulations indicate that CrO<sub>2</sub> monolayer is dynamically, thermally, and mechanically stable. The convex hull diagram of Cr—O systems shows the hull energy of the predicted CrO<sub>2</sub> layer is only 0.18 eV, further confirming the structural stability and large possibility for experimental fabrication. More importantly, the electronic and magnetic properties of CrO<sub>2</sub> monolayer demonstrate that it is a two-dimensional ferromagnetic half-metal with wide band gap. Five <i>d</i> suborbitals are divided into E<sub>g</sub> and T<sub>2g</sub> orbitals because of the crystal field of Cr atom at the center of O tetrahedron, and the spin-polarization of E<sub>g</sub> orbitals make a major contribution to the moment around Cr atom. The ferromagnetic coupling along Cr-O-Cr chain is dominated by the superexchange interaction bridged by O 2p orbital, similar to the typical Mn-O-Mn superexchange model. The magnetic behavior of the Cr spin lattice in a CrO<sub>2</sub> monolayer is described by a two-dimensional Heisenberg model, in which the exchange coupling anisotropy is ignored and the single ion anisotropy is the main consideration. By solving the Heisenberg model using the Monte Carlo simulation method, the Curie temperature is determined to be over 400 K. The high Curie temperature ferromagnetism is rare in two-dimensional ferromagnetic materials and even rarer in semi-metallic materials, which makes it an ideal material for the fabrication of spintronic devices and the study of spin quantum effects.