Thickness Dependent Properties in Oxide Heterostructures Driven by Structurally Induced Metal–Oxygen Hybridization Variations. (15th March 2017)

• Record Type: Journal Article
• Authors: Liao, Zhaoliang; Gauquelin, Nicolas; Green, Robert J.; Macke, Sebastian; Gonnissen, Julie; Thomas, Sean; Zhong, Zhicheng; Li, Lin; Si, Liang; Van Aert, Sandra; Hansmann, Philipp; Held, Karsten; Xia, Jing; Verbeeck, Johan; Van Tendeloo, Gustaaf; Sawatzky, George A.; Koster, Gertjan; Huijben, Mark; Rijnders, Guus
• Is Part Of: Advanced functional materials. Volume 27:Number 17(2017)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2017-03-15
• Subjects: interfaces -- manganites -- metal–oxygen hybridization -- oxide heterostructures -- oxygen octahedral couplings; Materials -- Periodicals; Chemical vapor deposition -- Periodicals; 620.11
• DOI: 10.1002/adfm.201606717
• Languages: English
• ISSNs: 1616-301X

Abstract

Abstract : 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 La2/3 Sr1/3 MnO3 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. Abstract : Relaxation of oxygen‐2p and Mn‐3d orbital (p–d) hybridization is coupled to the layer‐dependent octahedral tilts within a La2/3 Sr1/3 MnO3 film driven by interfacial octahedral coupling. Enhanced Curie temperatures are achieved by reducing the octahedral tilting via interface structure engineering, demonstrating the central role of thickness‐dependent p–d hybridization in widely observed dimensionality effects present in correlated oxide heterostructures.