Abstract
Competing exchange interactions can give rise to varying degrees of frustration that manifest itself in noncollinear magnetic moment ordering or canonical geometric frustration in magnets with large ground-state degeneracies. Relieving this frustration has the potential to stabilize ground states inaccessible in the bulk. We demonstrate that heteroepitaxial lattice distortions can modify the strength of exchange interactions in thin films of the frustrated ferrimagnet, CuCr2O4. The reduction of magnetic frustration in CuCr2O4 through lattice distortions results in greater collinear spin ordering in CuCr2O4 thin films and an enhanced magnetization. We identify heteroepitaxial lattice distortions as a method to tune spin functionality and potentially lift ground-state degeneracies more broadly in frustrated magnets.