Emergence of robust half-metallic spin gap and a sizeable magnetic anisotropy in electron-doped Ca[formula omitted]FeOsO[formula omitted

Abstract

Half-metallic materials having a large band gap (Eg) along with giant magnetocrystalline anisotropy energy (MAE) have been proposed to be crucial for the development of magnetic tunnel junctions. Herein, electron-doped Ca2FeOsO6 (CFOO) double perovskite oxide is investigated by employing ab-initio calculations with the inclusion of Hubbard U and spin–orbit coupling effects. Electron doping is realized by introducing Co+2/Ni+2 ion with 3d7 (t2g3↑t2g2↓eg2↑eg0↓)/3d8 (t2g3↑t2g3↓eg2↑eg0↓) configuration at Fe+33d5 (t2g3↑t2g0↓eg2↑eg0↓) site. The thermodynamical, mechanical, and dynamical stability of these motifs for determining the synthesis feasibility at ambient conditions is established by calculating the formation energetics, elastic constants, and phonon band structure, respectively. The undoped CFOO system displays a ferrimagnetic Mott-insulating behavior due to a strong antiferromagnetic coupling between Fe and Os ions. On the other hand, electron doping induces half metallicity in CFOO, where extra electrons provided by TM-dopants produce a repulsion in the partially filled Os t2g3↓ spin-minority channel. As a consequence, the Os bands near the Fermi level are shifted to higher energetics; resulting in a conducting nature for the doped motifs. Therefore, Os ion remains in the mixed formal valence states of Os+5 and Os+6/Os+7, which reduces the moments as well. Most remarkably, a large Eg of 1.26/1.65 eV exists in the spin-majority channel of Co/Ni-doped structure, which is highly desired to effectively suppress the spin-flipping and affirm the large mean free path for spins along with a high spin-filtering response. Our results also demonstrated that the half metallicity of the studied TM-doped CFOO is robust and can be preserved under a reasonable magnitude of biaxial strains ([110]). Additionally, a sizeable MAE constant of ∼×107 erg/cm3 indicates that these materials could be potential candidates for the data storage devices.