Large orbital polarization in nickelate-cuprate heterostructures by dimensional control of oxygen coordination

Artificial heterostructures composed of dissimilar transition metal oxides provide unprecedented opportunities to create remarkable physical phenomena. Here, we report a means to deliberately control the orbital polarization in LaNiO(3) (LNO) through interfacing with SrCuO(2) (SCO), which has an infinite-layer structure for CuO(2). Dimensional control of SCO results in a planar-type (P–SCO) to chain-type (C–SCO) structure transition depending on the SCO thickness. This transition is exploited to induce either a NiO(5) pyramidal or a NiO(6) octahedral structure at the SCO/LNO interface. Consequently, a large change in the Ni d orbital occupation up to ~30% is achieved in P–SCO/LNO superlattices, whereas the Ni e(g) orbital splitting is negligible in C–SCO/LNO superlattices. The engineered oxygen coordination triggers a metal-to-insulator transition in SCO/LNO superlattices. Our results demonstrate that interfacial oxygen coordination engineering provides an effective means to manipulate the orbital configuration and associated physical properties, paving a pathway towards the advancement of oxide electronics.