Synthesis and properties of charge-ordered thallium halide perovskites, CsTl1+0.5Tl3+0.5X3 (X = F, Cl)- theoretical precursors for superconductivity?
M. Retuerto, T. Emge, J. Hadermann, P. W. Stephens, M. R. Li, Z. P. Yin, M. Croft, A. Ignatov, S. J. Zhang, Z. Yuan, C. Jin, J. W. Simonson, M. C. Aronson, A. P… 展开作者
M. Retuerto, T. Emge, J. Hadermann, P. W. Stephens, M. R. Li, Z. P. Yin, M. Croft, A. Ignatov, S. J. Zhang, Z. Yuan, C. Jin, J. W. Simonson, M. C. Aronson, A. Pan, D. N. Basov, G. Kotliar, M. Greenblatt
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Accepted for publication in Chemistry of Materials; Publication Date (Web): September 18, 2013
Recently CsTlCl3 and CsTlF3 perovskites were theoretically predicted to be potential superconductors if they are optimally doped. The synthesis of these two compounds, together with a complete characterization of the samples are reported. CsTlCl3 is obtained as orange crystals in two different polymorphs: a tetragonal (I4/m) and a cubic (Fm-3m) phase. CsTlF3 is formed as a light brown powder, also as a double cubic perovskite (Fm-3m). In all three CsTlX3 phases Tl1+ and Tl3+ were located in two different crystallographic positions that accommodate their different bond lengths. In CsTlCl3 some Tl vacancies are found in the Tl1+ position. The charge ordering between Tl1+ and Tl3+ was confirmed by x-ray absorption and Raman spectroscopy. The Raman spectroscopy of CsTlCl3 under high pressure (58 GPa) did not indicate any phase transition to a possible single Tl2+ state. However, the highly insulating material becomes less resistive with increasing high pressure, while undergoing a change in the optical properties, from transparent to deeply opaque red, indicative of a decrease of the band gap. The theoretical design and experimental validation of the existence of CsTlF3 and CsTlCl3 cubic perovskites is the necessary first step in confirming the theoretical prediction of superconductivity in these materials.
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Ben Gurion University of the Negev（内盖夫本-古里安大学）；The Alexander Kofkin Faculty of Engineering, Bar Ilan University（巴伊兰大学亚历山大·科夫金工程学院）；Ilse Katz Institute for Nanoscale Science and Technology, Ben-Gurion University of the Negev（内盖夫本-古里安大学伊尔斯·卡茨纳米科学与技术研究所）；Weizmann Institute of Science（魏茨曼科学研究所）
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Helmholtz-Zentrum Berlin für Materialien und Energie（亥姆霍兹柏林材料与能源中心）；Department of Chemistry, Humboldt-Universität zu Berlin（柏林洪堡大学化学系）；Department of Interface Science, Fritz Haber Institute of the Max Planck Society（马克斯·普朗克学会弗里茨·哈伯研究所界面科学部）；Faculty of Electrical Engineering and Computer Science, Technical University Berlin（柏林工业大学电气与计算机工程学院）
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Julius-Maximilian University of Würzburg（维尔茨堡大学）；Institute for Scintillation Materials, National Academy of Sciences of Ukraine（乌克兰国家科学院闪烁材料研究所）；Paderborn University（帕德博恩大学）；Universidade Estadual de Campinas-UNICAMP（坎皮纳斯州立大学）
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CIC nanoGUNE（纳米材料中心）；Fisika Saila, Centro Fı́sica Materiales CSIC-UPV/EHU（巴斯克国家研究委员会-巴斯克国立大学物质物理中心物理系）；Centre for Advanced Materials and Technologies (CEZAMAT), Warsaw University of Technology（华沙理工大学先进材料与技术中心）；Key Laboratory for Special Functional Materials of Ministry of Education, School of Nanoscience and Materials Engineering, Henan University（河南大学纳米科学与工程学部委部省共建特殊功能材料重点实验室）；Instituto de Ciencia de los Materiales (ICMUV), Universitat de Valencia（瓦伦西亚大学材料科学研究所）；Donostia International Physics Center（圣塞巴斯蒂安国际物理中心）；Ikerbasque, Basque Foundation for Science（伊克尔巴斯科，巴斯克科学基金会）；Polymat, University of the Basque Country UPV/EHU（巴斯克国立大学聚合物材料研究中心）；BCMaterials, Basque Center for Materials, Applications and Nanostructures, UPV/EHU Science Park（巴斯克材料、应用与纳米结构中心）
