Reversible Control of Physical Properties via an Oxygen-Vacancy-Driven Topotactic Transition in Epitaxial La0.7Sr0.3MnO3-δ Thin Films

被引:75
作者
Cao, Lei [1 ,2 ]
Petracic, Oleg [1 ,2 ]
Zakalek, Paul [1 ,2 ]
Weber, Alexander [3 ]
Ruecker, Ulrich [1 ,2 ]
Schubert, Juergen [4 ]
Koutsioubas, Alexandros [3 ]
Mattauch, Stefan [3 ]
Brueckel, Thomas [1 ,2 ,3 ]
机构
[1] Forschungszentrum Julich, JARA FIT, Julich Ctr Neutron Sci JCNS 2, D-52425 Julich, Germany
[2] Forschungszentrum Julich, JARA FIT, Peter Grunberg Inst PGI 4, D-52425 Julich, Germany
[3] Forschungszentrum Julich, Heinz Maier Leibnitz Zentrum MLZ, JCNS, D-85748 Garching, Germany
[4] Forschungszentrum Julich, JARA Fundamentals Future Informat Technol, Peter Grunberg Inst PGI9 IT, D-52425 Julich, Germany
关键词
brownmillerite; La0.7Sr0.3MnO3; films; magnetism; oxygen vacancy ordering; polarized neutron reflectometry; MECHANISMS; REDUCTION; SURFACE; CATION;
D O I
10.1002/adma.201806183
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The vacancy distribution of oxygen and its dynamics directly affect the functional response of complex oxides and their potential applications. Dynamic control of the oxygen composition may provide the possibility to deterministically tune the physical properties and establish a comprehensive understanding of the structure-property relationship in such systems. Here, an oxygen-vacancy-induced topotactic transition from perovskite to brownmillerite and vice versa in epitaxial La0.7Sr0.3MnO3-delta thin films is identified by real-time X-ray diffraction. A novel intermediate phase with a noncentered crystal structure is observed for the first time during the topotactic phase conversion which indicates a distinctive transition route. Polarized neutron reflectometry confirms an oxygen-deficient interfacial layer with drastically reduced nuclear scattering length density, further enabling a quantitative determination of the oxygen stoichiometry (La0.7Sr0.3MnO2.65) for the intermediate state. Associated physical properties of distinct topotactic phases (i.e., ferromagnetic metal and antiferromagnetic insulator) can be reversibly switched by an oxygen desorption/absorption cycling process. Importantly, a significant lowering of necessary conditions (temperatures below 100 degrees C and conversion time less than 30 min) for the oxygen reloading process is found. These results demonstrate the potential applications of defect engineering in the design of perovskite-based functional materials.
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页数:7
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