In Quest of a Ferromagnetic Insulator: Structure-Controlled Magnetism in Mg-Ti-O Thin Films

Ferromagnetic insulator thin films can convey information by spin waves, avoiding charge displacement and Eddy current losses. The sparsity of high-temperature insulating ferromagnetic materials hinders the development of spin-wave-based devices. Stoichiometric magnesium titanate, MgTiO₃, has an electronic-energy-band structure in which all bands are either full or empty, being a paramagnetic insulator. The MgTiO₃ ilmenite consists of ordered octahedra and a cation network in which one-third of the octahedra are vacant, one-third host magnesium, and one-third titanium. By giving up these characteristics, a rich variety of different magnetic structures can be formed. Our experiments and electronic-energy-band-structure computations show that the magnetic and electric properties of Mg-Ti-O films can drastically be changed and controlled by Mg- and Ti-cation arrangement and abundancy in the octahedra. Insulating titanium- and semiconducting magnesium-rich films exhibited reversible magnetization up to elevated temperatures. The presence and origin of the insulating phase with reversible magnetization, assigned to ferromagnetic ordering, is not apparent. The expectation, based on the well-established rules set by Goodenough and Kanamori, is paramagnetic or antiferromagnetic ordering. We show that ferro- and paramagnetic phases, possessing the same stoichiometry, can be obtained by merely rearranging the cations, thus allowing defect-free interfaces in multilayer structures.