High spin polarization, large perpendicular magnetic anisotropy and room-temperature ferromagnetism by biaxial strain and carrier doping in Janus MnSeTe and MnSTe

Abstract

The emerging two-dimensional (2D) Janus systems with broken symmetry provide a new platform for designing ultrathin multifunctional spintronic materials. Recently, based on experimental monolayer MnSe₂, ferromagnetism was predicted in Janus MnXY (X ≠ Y = S, Se, Te) monolayers; however, they exhibit low Curie temperatures and small magnetic anisotropic energies. To improve the Curie temperature and magnetic anisotropy, herein, we systemically explore the stability and electronic and magnetic properties of Janus MnSeTe and MnSTe monolayers under strain and carrier-doping using first-principles calculations and Monte Carlo simulations. It is found that both MnSeTe and MnSTe monolayers possess robustly high spin polarization with rational strain and carrier-doping. Both tensile strain and hole doping strengthen the ferromagnetic super-exchange interactions of the two nearest Mn atoms mediated by chalcogen atoms and exceedingly improve the perpendicular magnetic anisotropic energies (by up to 3.1 meV per f.u. for MnSeTe and 2.0 meV per f.u. for MnSTe). The Te-5p intraorbital hybridizations contributed to the main magnetic anisotropy. More remarkably, the tensile strain and hole doping collectively increase the Curie temperatures of MnSeTe and MnSTe to above and near room temperature (345 and 290 K, respectively). The present study reveals that Janus MnSeTe and MnSTe monolayers with robustly high spin polarization, room-temperature ferromagnetism and large perpendicular magnetic anisotropy are promising candidates for ultrathin multifunctional spintronic materials. This study will be of great interest for further experimental and theoretical explorations of 2D Janus manganese dichalcogenides.