Bilayer hexagonal structure MnN2 nanosheets with room-temperature ferromagnetic half-metal behavior and a tunable electronic structure

Abstract

Two-dimensional (2D) layered materials have atomically thin thickness and outstanding physical properties, attracting intensive research in the past year. As one of these materials, a 2D magnet is an ideal platform for fundamental physics research and magnetic device development. Recently, a non-MoS₂-type geometry was found to be more favorable in 2D transition-metal dinitrides. In this work, driven by this new configuration, we perform a comprehensive first-principles study on the bilayer hexagonal structure of 2D manganese dinitrides. Our results show that 2D MnN₂ is a ferromagnetic half-metal at its ground state with 100% spin-polarization ratio at the Fermi energy level. The phonon spectrum calculation and ab initio molecular dynamics simulation show that the 2D MnN₂ crystal has a high thermodynamic stability and its 2D lattice can be retained at room-temperature. Monte Carlo simulations based on the Heisenberg model predict a Curie temperature of over 563 K and its electronic properties can be regulated by biaxial strain. The half-metallic states are mainly contributed by Mn d orbitals, and the magnetic exchange of the system mainly comes from the Mn–N–Mn super-exchange. The p–d orbital hybridization will provide a small antiparallel magnetic moment of N atoms, and the p-orbital dangling bond can be eliminated by oxidation to enhance the total magnetic moment of the system. The study of magnetic anisotropy energy indicates that the easy magnetization axis is in-plane and hybridization between Mn d_yz and d_z² orbitals gives the largest magnetic anisotropy contribution. In view of these results, we consider that novel 2D MnN₂ is one of the most promising two-dimensional materials for nano-spintronic applications.