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Hybrid perovskite X-ray detectors with enhanced radioluminescence via thermally activated delayed fluorescence

热激活延迟荧光增**型钙钛矿闪烁体及其X射线探 测器

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Abstract

Recently, metal halide perovskites have received great attention for detecting ionizing radiation. Perovskite-based photodetectors and scintillators have been successfully implemented for X-ray and γ-ray detection due to their high attenuation coefficient and excellent optoelectronic properties. However, relatively thick absorbing layers are required for the complete absorption of X-ray photons, which are very challenging to fabricate with solution processes. In this work, we designed hybrid devices coupled with excellent perovskite photodiodes to utilize the incident X-rays fully. Considering the heavy reabsorption of the perovskite layers, we blended CsPbBr3 with a Cu(I)-containing thermally activated delayed fluorescent complex (MAC*)Cu(Cz) to achieve down-conversion luminescence effectively to maximize the radioluminescence quantum efficiency, and we also found a faster afterglow compared with the commercial scintillators. Furthermore, we systematically investigated the performance metrics of the CsPbIBr2 photodiodes and scintillator films. The hybrid devices demonstrated significantly improved X-rays sensitivity, indicating potential for X-ray detection and imaging.

摘要

金属卤化物钙钛矿材料具有极高的射线衰减系数和优良的光电 性能, 基于其制备的光电探测器和闪烁体已成功用于X射线和γ-射线探 测. 然而, 充分吸收高能射线需要相对较厚的光吸收层, 但所需的厚度 对于溶液法制备的钙钛矿薄膜来说很难达到. 在这项工作中, 我们设计 了一种复合型器件, 其不需要厚的钙钛矿吸收层, 而是利用高荧光效率 的钙钛矿闪烁体和性能优良的钙钛矿薄膜光电探测器充分吸收和利用 X射线, 从而提高X射线探测性能. 而考虑到钙钛矿闪烁体严重的自吸 收, 我们将CsPbBr3与含Cu(I)的热激活延迟荧光配合物(MAC*)Cu(Cz) 混合, 有效地实现了下转换发光, 最大限度地提高了辐射发光量子效率. 与商业闪烁体相比, 混合闪烁体还实现了更短的余辉. 此外, 我们系统 地研究对比了CsPbIBr2探测器以及复合型探测器的性能指标, 发现复 合型探测器对X射线的探测灵敏度有显著提高, 并且能够实现在X射线 下清晰的成像. 这项工作为提高X射线探测性能提供了一种新的思路, 在应用层面具有巨大的潜力.

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (61875154 and 52022071), the Natural Science Foundation of Jiangsu Province, China (BK20190214), the National Key R&D Program of China (2020YFB2008800), and China Postdoctoral Science Foundation (2021M702513).

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  1. These authors contributed equally to this work.

Authors and Affiliations

  1. Key Lab of Artificial Micro- and Nano-Structures of Ministry of Education of China, School of Physics and Technology, Wuhan University, Wuhan, 430072, China

    Yalun Xu  (许亚伦), Jiali Peng  (彭家丽), Fang Yao  (姚方), Ruiming Li  (**睿明) & Qianqian Lin  (林乾乾)

  2. Department of Chemistry, Hubei Key Lab on Organic and Polymeric Optoelectronic Materials, Wuhan University, Wuhan, 430072, China

    Ao Ying  (应翱), Yao Tan  (谭瑶) & Shaolong Gong  (龚少龙)

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  1. Yalun Xu  (许亚伦)
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  2. Ao Ying  (应翱)
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  4. Fang Yao  (姚方)
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  7. Shaolong Gong  (龚少龙)
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  8. Qianqian Lin  (林乾乾)
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Contributions

Xu Y and Ying A performed the experiments and cowrote the paper. Peng J and Yao F helped analyze the data and reviewed the paper. Li R and Tan Y helped the preparation and characterization of materials. Lin Q and Gong S supervised the study. All authors contributed to the general discussion.

Corresponding authors

Correspondence to Shaolong Gong  (龚少龙) or Qianqian Lin  (林乾乾).

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Conflict of interest

The authors declare that they have no conflict of interest.

Supplementary information

Experimental details and supporting data are available in the online version of the paper.

Yalun Xu received his bachelor’s degree in materials physics at Wuhan University in 2018. Since 2018, he has been a PhD student in the group of Prof. Qianqian Lin at the School of Physics and Technology, Wuhan University. His research interests include material characterization, semiconductor physics and opto-electronic materials.

Ao Ying is a PhD student at Hubei Key Lab on Organic and Polymeric Optoelectronic Materials, Wuhan University. His research focuses on the optoelectronic materials and devices, mainly in the design, synthesis, and photophysics of luminescent coinage-metal complexes.

Shaolong Gong received his PhD degree in materials physics and chemistry from Wuhan University in 2012. After the two-year postdoctoral study at the University of Toronto, he joined the faculty of Wuhan University as an associate professor in 2014 and was promoted to a full professor in 2020. His current research interests are centered on the molecular design and synthesis of new-generation organic emitters and luminescent coinage metal complexes for organic optoelectronic devices.

Qianqian Lin is currently a professor of materials physics at the School of Physics and Technology, Wuhan University. He received his PhD degree from The University of Queensland, Australia, in 2016. After a postdoctoral position at the Clarendon Laboratory, University of Oxford, UK, he joined Wuhan University in 2017. His research interests include characterizations of advanced functional materials, chalcogenides and perovskite/organic opto-electronic devices.

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Xu, Y., Ying, A., Peng, J. et al. Hybrid perovskite X-ray detectors with enhanced radioluminescence via thermally activated delayed fluorescence. Sci. China Mater. 66, 724–732 (2023). https://doi.org/10.1007/s40843-022-2193-6

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