Infinite-layer/perovskite oxide heterostructure-induced high-spin states in SrCuO₂/SrRuO₃ bilayer films

Heterostructures composed of dissimilar oxides with different properties offer opportunities to develop emergent devices with desired functionalities. A key feature of oxide heterostructures is interface electronics and orbital reconstructions. Here, we combined infinite-layered SrCuO₂ and perovskite SrRuO₃ into heterostructures. A rare high spin state as large as 3.0 <i>μ</i>_B f.u^-1 and an increase in Curie temperature by 12 K are achieved in an ultrathin SrRuO₃ film capped by a SrCuO₂ layer. Atomic-scale lattice imaging shows the uniform CuO₂-plane-to-RuO₅-pyramid connection at the interface, where the regularly arranged RuO₅ pyramids were elongated along the out-of-plane direction. As revealed by theoretical calculations and spectral analysis, these features finally result in an abnormally high spin state of the interfacial Ru ions with highly polarized e_g orbitals. The present work demonstrates that oxygen coordination engineering at the infinite-layer/perovskite oxide interface is a promising approach towards advanced oxide electronics.