Spin canting and orbital order in spinel vanadate thin films

We report on the epitaxial film growth and characterization of CoV2O4, a near-itinerant spinel vanadate, grown on (001) SrTiO3. The symmetry lowering of the unit cell from cubic in the bulk to orthorhombic in the films results in dramatic differences in the magnetic anisotropy compared to bulk, as determined from structural and magnetic characterization. Bulk cubic CoV2O4 has been found to defy predictions by showing orbital degeneracy seemingly lasting to very low temperatures, with only small anomalies in magnetization and neutron experiments signaling a possible spin/orbital glass transition at T=90 K. In epitaxial thin films presented in this paper, structurally tuning the CoV2O4 away from cubic symmetry leads to a completely different low temperature noncollinear ground state. Via magnetization and neutron scattering measurements we show that the 90-K transition is associated with a major spin reorientation away from the ferrimagnetic easy axis [001] to the [110] direction. Furthermore, the V spins cant away from this direction with extracted perpendicular moments providing evidence of a larger canting angle compared to bulk. This result indicates that compressive strain pushes the system deeper into the insulating state, i.e., away from the localized-itinerant crossover regime.