Herein, a low-temperature thermal decomposition method is utilized to grow new stable tetragonal Fe3O4-based thick ferrite films. The tetragonal Fe3O4-based film possesses high saturation magnetization of ∼800 emu/cm3. Doping with approximately 10% Co results in a high-energy product of ∼10.9 MGOe with perpendicular magnetocrystalline anisotropy, whereas doping with Ni increases electrical resistivity by a factor of 6 and retains excellent soft magnetic properties (high saturation magnetization and low coercivity). A combined experimental and first-principles study reveals that carbon interstitials (CiB) and oxygen vacancies (VO) form CiB-VO pairs which stabilize the tetragonal phase and enhance saturation magnetization. The magnetization enhancement is further attributed to local ferromagnetic coupling between FeA and FeB induced by CiB-VO pairs in a tetragonal spinel ferrite lattice.
Keywords: ferrite; first-principles calculations; high magnetization; tetragonal film; thermal decomposition.