Thickness Dependent Properties in Oxide Heterostructures Driven by Structurally Induced Metal–Oxygen Hybridization Variations

Zhaoliang Liao, N. Gauquelin, R.J. Green, S. Macke, J. Gonissen, S. Thomas, Z. Zhong, Lin Li, L. Si, S. van Aert, P. Hansmann, K. Held, J. Xia, J. Verbeeck, G. van Tendeloo, G.A. Sawatzky, Gertjan Koster, Mark Huijben, Guus Rijnders

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Thickness-driven electronic phase transitions are broadly observed in different types of functional perovskite heterostructures. However, uncertainty remains whether these effects are solely due to spatial confinement, broken symmetry, or rather to a change of structure with varying film thickness. Here, this study presents direct evidence for the relaxation of oxygen-2p and Mn-3d orbital (p–d) hybridization coupled to the layer-dependent octahedral tilts within a La2/3Sr1/3MnO3 film driven by interfacial octahedral coupling. An enhanced Curie temperature is achieved by reducing the octahedral tilting via interface structure engineering. Atomically resolved lattice, electronic, and magnetic structures together with X-ray absorption spectroscopy demonstrate the central role of thickness-dependent p–d hybridization in the widely observed dimensionality effects present in correlated oxide heterostructures.
Original languageEnglish
Article number1606717
Number of pages9
JournalAdvanced functional materials
Issue number17
Publication statusPublished - 4 May 2017


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