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Published Online October 11, 2007
Science DOI: 10.1126/science.1149338

Research Articles

Submitted on August 16, 2007
Accepted on October 2, 2007

Orbital Reconstruction and Covalent Bonding at an Oxide Interface

J. Chakhalian 1*, J. W. Freeland 2, H.-U. Habermeier 3, G. Cristiani 3, G. Khaliullin 3, M. van Veenendaal 4, B. Keimer 3

1 University of Arkansas, Fayetteville, AR 72701, USA.; Max Planck Institute for Solid State Research, D-70569 Stuttgart, Germany.
2 Advanced Photon Source, Argonne National Laboratory, Argonne, IL 60439, USA.
3 Max Planck Institute for Solid State Research, D-70569 Stuttgart, Germany.
4 Advanced Photon Source, Argonne National Laboratory, Argonne, IL 60439, USA.; Department of Physics, Northern Illinois University, Dekalb, IL 60115, USA.

* To whom correspondence should be addressed.
J. Chakhalian , E-mail: jchakhal{at}uark.edu

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)Ba2Cu3O7 and metallic La2/3Ca1/3MnO3 by resonant x-ray spectroscopy. A charge of about -0.2e 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 CuO2 layers. In particular, the Cu d3z2-r2 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 determining the physical properties of oxide heterostructures.


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Science. ISSN 0036-8075 (print), 1095-9203 (online)