Tailoring magnetism in spinel vanadate CoV₂O₄epitaxial thin films

Near itinerant cubic bulk CoV₂O₄is at variance with other spinel vanadates by not showing orbital ordering down to low temperature, albeit it displays fragile anomalies related to spin, and lattice structure, signaling a spin/orbital glass transition around 95 K. We investigate tetragonal-like epitaxial CoV₂O₄films on SrTiO₃and (La_0.3Sr_0.7)(Al_0.65Ta_0.35)O₃substrates that exhibit pronounced signature of spin reorientation transition from toa/bplane around 90 K unlike its bulk counterpart. Using in-plane and out-of-plane magnetic measurements, we demonstrate the intricate link between Co²⁺and V³⁺sublattice magnetizations that give rise to anisotropic magnetic switching. In-plane magnetic measurements reveal a wasp-waist shapedM(H) loop below reorientation transition temperature, while the out-of-plane follows antiferromagnet-likeM(H) response. The wasp-waist shaped feature could be linked to in-plane spin-canted (anti)ferromagnetism induced by canting away of V-spins away from antiferromagnetically coupled Co-spin direction below reorientation transition temperature. Further, we uncover the evidence for slow relaxation over a period of ∼10⁴ s at 20 K and memory effect that indicates the possible existence for magnetic glassy phase in the low temperature regime. Using epitaxial strain as a control knob, our results inspire future study to manipulate orbital states, spin texture and itinerant electron character in tailored CoV₂O₄films away from cubic lattice symmetry.