Abstract
Zero-dimensional metal halide perovskites have captured intense research interest owing to their unique optoelectronic properties. Particularly, metal halides with the ns2 electronic configuration are of great interest owing to the high-temperature sensitivity of their photoluminescence, which could be applied to remote optical thermometry (ROT). Herein, all-inorganic and lead-free halide perovskite Te4+-doped Cs2InCl5·H2O single crystals (SCs) were prepared through the hydrothermal method and showed a strong temperature dependence of photoluminescence lifetime. Upon Te4+ doping, the nonemissive Cs2InCl5·H2O SC exhibits a bright orange emission at 660 nm with a wide full width at half maximum of 180 nm. The strong phonon-exciton coupling promotes the formation of self-trapped excitons in the soft lattice of the zero-dimensional Te4+-doped Cs2InCl5·H2O SC. The Te4+ ions with the 5s2 electronic configuration endow the Te4+-doped Cs2InCl5·H2O SC with a strong temperature-dependent photoluminescence lifetime. This SC reaches a maximum specific sensitivity of 0.062K−1 at 320 K, thereby showing the potential advantages of indium-based metal halide perovskites in ROT applications.
摘要
本文设计合成了一种Te4+离子掺杂的Cs2InCl5·H2O单晶, 该单晶在紫外光激发下发射明亮橙光. 未掺杂的Cs2InCl5·H2O单晶几乎没有发光现象, 但Te4+掺杂的Cs2InCl5·H2O单晶, 发射峰位于660 nm, 并伴随着大的Stokes位移和宽的发光半峰宽(180 nm). 结合变温荧光光谱以及飞秒瞬态吸收光谱等表征, 揭示了其发光机理为自陷激子发光. 零维结构中的强电声耦合以及软晶格有利于形成并稳定自陷激子. 特别地, 由于Te4+离子的最外层电子结构为5s2, 对温度变化较为灵敏, Te4+离子掺杂的Cs2InCl5·H2O单晶的发光寿命表现出了非常强的温度依赖性, 发光寿命从80 K下的6 μs缩短至380 K下的19 ns, 320 K处的相对灵敏度达到0.062 K−1, 可以与传统稀土基光学测温材料相媲美. 据我们所知, 这是首次将铟基金属卤化物钙钛矿单晶应用于光学测温, 将为设计合成新型多功能响应的金属卤化物钙钛矿发光材料提供借鉴意义.
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Acknowledgements
This work was supported by the National Natural Science Foundation of China (U2001214), the Natural Science Foundation of Guangdong Province (2019B1515120050), and the Fundamental Research Funds for the Central Universities.
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Author contributions Kuang DB and Wei JH designed and carried out the experiments. Wei JH and Ou WT performed the material preparation, characterization, and data analysis. Liao JF and Luo JB helped with the TA measurement and data analysis and revised the manuscript. All authors participated in discussing the data and writing the manuscript.
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Jun-Hua Wei received her BS degree from Sun Yatsen University (SYSU) in 2018, and she is currently a PhD candidate advised by Professor Dai-Bin Kuang at the School of Chemistry, SYSU. Her current research interests focus on multifunctional and efficient lightemitting metal halide perovskite.
Dai-Bin Kuang is a professor at the School of Chemistry, SYSU. Dr. Kuang received his PhD degree from SYSU in 2003. He worked as a postdoctoral researcher at the Max Planck Institute of Colloids and Interfaces (Germany) from 2003 to 2004 and then at the Ecole Polytechnique Fédérale de Lausanne (Switzerland) from 2004 to 2008. His current research interests are in the field of new energy materials, focusing on light-emitting metal halide perovskite, perovskite photodetectors, photocatalysis, and photoelectrochemical cells.
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Wei, JH., Luo, JB., Liao, JF. et al. Te4+-doped Cs2InCl5·H2O single crystals for remote optical thermometry. Sci. China Mater. 65, 764–772 (2022). https://doi.org/10.1007/s40843-021-1792-1
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DOI: https://doi.org/10.1007/s40843-021-1792-1