Depth‐Resolved Modulation of Metal–Oxygen Hybridization and Orbital Polarization across Correlated Oxide Interfaces

다국어 초록 (Multilingual Abstract)

Interface‐induced modifications of the electronic, magnetic, and lattice degrees of freedom drive an array of novel physical properties in oxide heterostructures. Here, large changes in metal–oxygen band hybridization, as measured in the oxygen ligand hole density, are induced as a result of interfacing two isovalent correlated oxides. Using resonant X‐ray reflectivity, a superlattice of SrFeO3 and CaFeO3 is shown to exhibit an electronic character that spatially evolves from strongly O‐like in SrFeO3 to strongly Fe‐like in CaFeO3. This alternating degree of Fe electronic character is correlated with a modulation of an Fe 3d orbital polarization, giving rise to an orbital superstructure. At the SrFeO3/CaFeO3 interfaces, the ligand hole density and orbital polarization reconstruct in a single unit cell of CaFeO3, demonstrating how the mismatch in these electronic parameters is accommodated at the interface. These results provide new insight into how the orbital character of electrons is altered by correlated oxide interfaces and lays out a broadly applicable approach for depth‐resolving band hybridization.
Resonant X‐ray reflectivity is used to quantitatively measure changes in band hybridization across transition metal oxide interfaces. Spatially determining the degree of metal versus oxygen character in a superlattice of SrFeO3/CaFeO3 reveals how interfaces can alter the orbital character of valence electrons and further reveal a new class of oxide interfacial reconstructions, that of metal–oxygen hybridization.