Abstract
Oxygen usually plays crucial roles in tuning the phase structures and functionalities of complex oxides such as high temperature superconductivity, colossal magnetoresistance, catalysis, etc. Effective and considerable control of the oxygen content in those functional oxides could be highly desired. Here, using perovskite manganite (La0.5Sr0.5)MnO3 as a paradigm, we develop a new pathway to synthesize the epitaxial thin films assisted by an in-situ chemical process, where the oxygen content can be precisely controlled by varying oxidative activity tuned by the atmospheric temperature (Tatm) during the growth. A hidden metal-insulator transition (MIT) emerges due to the phase competition, which is never shown in the phase diagram of this classic manganite. The oxygen-mediated interaction between Mn ions together with the change of carrier density might be responsible for this emerging phase, which is compatible with the results of first-principle calculations. This work demonstrates that, apart from traditional cation doping, a precise modulation of anion (O2−, S2−, etc.) may provide a new strategy to control phase structures and functionalities of epitaxial compound thin films.
摘要
氧在调节复杂氧化物中的相结构和功能方面扮演着重要的角色, 比如高温超导体、 庞磁电阻、 催化等, 人们急需在这些功能氧化物中实现有效且可控的氧含量调控. 在此工作中我们通过改变气体氛围温度来精确的调控氧化活性, 从而实现一种新的化学辅助的高质量外延薄膜的制备方法. 以钙钛矿锰氧化物La0.5Sr0.5MnO3(LSMO)为例, 通过调控薄膜样品中氧的化学计量比, 我们首次发现了该体系中隐藏的由相竞争产生的金属-绝缘体转变. 氧组分引起的Mn离子间的交换相互作用以及载流子浓度的变化可能是此相转变产生的原因, 这与第一性原理计算十分符合. 不同于传统的阳离子掺杂, 有效的阴离子(O2−, S2−等)调节提供了一种新的实现复杂氧化物外延薄膜中调控相结构和功能的技术手段.
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Acknowledgements
This work was financially supported by the National Key Research and Development Program of China (2016YFA0302300). Zhang J also acknowledges the support from the National Natural Science Foundation of China (51332001) and the Fundamental Research Funds for the Central Universities (2017EYT26).
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Chuangye Song obtained his Bachelor’s degree in physics from Zhengzhou University in 2014. After that, he continued his education as a PhD candidate under the supervision of Prof. Jinxing Zhang at the Department of Physics, Beijing Normal University. His research interest now is the epitaxial growth of correlated-electron oxide film and the surface novel electronic phases at atomic scale by scanning tunneling microscopy in extreme conditions.
Jinxing Zhang obtained his PhD from Hong Kong Polytechnic University in 2009 under the supervision of Prof. Helen Chan. After that he continued his research work at the Department of Physics of University of California, Berkeley as a post-doc scholar at Professor R. Ramesh’s group. In 2012, he joined the Department of Physics, Beijing Normal University as a professor. The central goal of Zhang’s group is the pursuit of the emerging phenomena and exotic physical behaviors behind the coupling and control of multiple order parameters (e.g., lattice, spin, orbital, charges) at a reduced dimension. His team is striving to create a bridge between those fundamentally scientific discoveries in functional nano-systems and future possible applications such as sensing, actuation, data storage, energy conversion, quantum manipulation, etc.
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Song, C., Malik, I.A., Li, M. et al. Hidden metal-insulator transition in manganites synthesized via a controllable oxidation. Sci. China Mater. 62, 577–585 (2019). https://doi.org/10.1007/s40843-018-9344-5
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DOI: https://doi.org/10.1007/s40843-018-9344-5