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, we present 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.
@article{arxiv.1701.07930,
title = {Thickness dependent properties in oxide heterostructures driven by structurally induced metal-oxygen hybridization variations},
author = {Zhaoliang Liao and Nicolas Gauquelin and Robert J. Green and Sebastian Macke and Julie Gonnissen and Sean Thomas and Zhicheng Zhong and Lin Li and Liang Si and Sandra Van Aert and Philipp Hansmann and Karsten Held and Jing Xia and Johan Verbeeck and Gustaaf Van Tendeloo and George A. Sawatzky and Gertjan Koster and Mark Huijben and Guus Rijnders},
journal= {arXiv preprint arXiv:1701.07930},
year = {2017}
}