Orbital Reconstruction and Covalent Bonding at an Oxide Interface

Abstract

Orbital reconstructions and covalent bonding must be considered as important factors in the rational design of oxide heterostructures with engineered physical properties. We have investigated the interface between high-temperature superconducting (Y,Ca)Ba 2 Cu 3 O 7 and metallic La 0.67 Ca 0.33 MnO 3 by resonant x-ray spectroscopy. A charge of about –0.2 electron is transferred from Mn to Cu ions across the interface and induces a major reconstruction of the orbital occupation and orbital symmetry in the interfacial CuO 2 layers. In particular, the Cu d 3 z 2 – r 2 orbital, which is fully occupied and electronically inactive in the bulk, is partially occupied at the interface. Supported by exact-diagonalization calculations, these data indicate the formation of a strong chemical bond between Cu and Mn atoms across the interface. Orbital reconstructions and associated covalent bonding are thus important factors in determining the physical properties of oxide heterostructures.