High-Magnetization Tetragonal Ferrite-Based Films Induced by Carbon and Oxygen Vacancy Pairs

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 (C_i^B) and oxygen vacancies (V_O) form C_i^B-V_O pairs which stabilize the tetragonal phase and enhance saturation magnetization. The magnetization enhancement is further attributed to local ferromagnetic coupling between Fe_A and Fe_B induced by C_i^B-V_O pairs in a tetragonal spinel ferrite lattice.