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Cs2AgBiBr6 single-crystal X-ray detectors with a low detection limit

Nature Photonics volume 11, pages 726–732 (2017)Cite this article

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Abstract

Sensitive X-ray detection is crucial for medical diagnosis, industrial inspection and scientific research. The recently described hybrid lead halide perovskites have demonstrated low-cost fabrication and outstanding performance for direct X-ray detection, but they all contain toxic Pb in a soluble form. Here, we report sensitive X-ray detectors using solution-processed double perovskite Cs2AgBiBr6 single crystals. Through thermal annealing and surface treatment, we largely eliminate Ag+/Bi3+ disordering and improve the crystal resistivity, resulting in a detector with a minimum detectable dose rate as low as 59.7 nGyair s−1, comparable to the latest record of 0.036 μGyair s−1 using CH3NH3PbBr3 single crystals. Suppressed ion migration in Cs2AgBiBr6 permits relatively large external bias, guaranteeing efficient charge collection without a substantial increase in noise current and thus enabling the low detection limit.

X-ray detection is of great interest for a range of applications, including non-destructive product inspection, medical diagnostics and scientific research1,2,3. Compared with indirect strategies that involve conversion of X-ray into photons by scintillating phosphors and subsequent detection by photodiodes, direct conversion of X-ray radiation into an electrical signal enables higher spatial resolution and a simpler system configuration4. Among the various semiconductors explored for direct X-ray detection, the recently described organic–inorganic hybrid lead halide perovskites have demonstrated many exceptional properties, such as large X-ray attenuation coefficient, high carrier drift length per unit electric field (the μτ product, where μ is the carrier mobility and τ is the carrier lifetime), low-cost solution growth of single crystals (SCs), and easy integration with silicon electronics for imaging applications. Sensitive X-ray detectors employing either MAPbI3 (where MA is CH3NH3 +) thin films or MAPbBr3 SCs have been reported, achieving an impressive sensitivity of 2.1 × 104 µC Gyair −1 cm–2, significantly outperforming commercial α-Se X-ray detectors5,6,7. Very recently, Huang and co-workers reported a further breakthrough by monolithically integrating MAPbBr3 SCs with a Si substrate to obtain sensitive X-ray imaging7. In addition, energy-resolved gamma ray detection using FAPbI3 (where FA is NH2CH=NH2 +) SCs and Cs0.1FA0.9PbI2.8Br0.2 SCs have also been successfully demonstrated8,9.

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Fig. 1: Cs2AgBiBr6 perovskite properties.
Fig. 2: Optimization of Cs2AgBiBr6 SC.
Fig. 3: Performance of Cs2AgBiBr6 SC X-ray detector.
Fig. 4: Measured and calculated ionic migration in Cs2AgBiBr6 SCs.

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Acknowledgements

This work was supported financially by the Major State Basic Research Development Program of China (2016YFB0700700, 2016YFA0204000), the National Natural Science Foundation of China (91433105, 11674237, 51602211, 61501197, 61425001), the HUST Key Innovation Team for Interdisciplinary Promotion (2016JCTD111, 2017KFXKJC003) and the Natural Science Foundation of Jiangsu Province of China (grant no. BK20160299). The authors acknowledge the Analytical and Testing Center of HUST and facility support from the Center for Nanoscale Characterization and Devices, WNLO. Theoretical calculations were performed in TianHe-II of the National Supercomputer Center in Guangzhou. X. Miao and X. Yang at Huazhong University of Science and Technology and Z. Ning at ShanghaiTech University are thanked for help with measurements.

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Author notes

  1. Weicheng Pan, Haodi Wu, Jiajun Luo and Zhenzhou Deng contributed equally to this work.

Authors and Affiliations

  1. Wuhan National Laboratory for Optoelectronics (WNLO), Huazhong University of Science and Technology (HUST), 430074, Wuhan, China

    Weicheng Pan, Haodi Wu, Jiajun Luo, Cong Ge, Chao Chen, Guangda Niu, Lixiao Yin, Ying Zhou & Jiang Tang

  2. School of Optical and Electronic Information, Huazhong University of Science and Technology (HUST), 430074, Wuhan, China

    Weicheng Pan, Haodi Wu, Jiajun Luo, Cong Ge, Chao Chen, Guangda Niu, Lixiao Yin, Ying Zhou & Jiang Tang

  3. School of Information Engineering, Nanchang University, 330031, Nanchang, China

    Zhenzhou Deng

  4. School of Life Science and Technology, Huazhong University of Science and Technology, 430074, Wuhan, China

    Zhenzhou Deng & Qingguo Xie

  5. Soochow Institute for Energy and Materials InnovationS (SIEMIS), College of Physics, Optoelectronics and Energy & Collaborative Innovation Center of Suzhou Nano Science and Technology, Soochow University, 215006, Suzhou, China

    Xiaowei Jiang & Wan-Jian Yin

  6. Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province, Soochow University, 215006, Suzhou, China

    Xiaowei Jiang & Wan-Jian Yin

  7. Institute of Microstructure and Property of Advanced Materials, Beijing University of Technology, 100124, Beijing, China

    Lujun Zhu, Xiaoxing Ke & Manling Sui

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  1. Weicheng Pan
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Contributions

J.T. conceived and supervised the project. W.P., H.W., J.L., Z.D., G.N. and J.T. designed the experiments and analysed the data. W.P., H.W. and J.L. carried out most experiments regarding material preparation and characterizations, as well as device optimization. Z.D. carried out X-ray source building and initial detector performance characterization. X.J. and W.-J.Y. performed theoretical simulations and analysed the results. Q.X. provided the facility for X-ray detector measurements and some consultation. C.G., C.C. and Y.Z. assisted with device optimization and data analysis. L.Z., X.K. and M.S. carried out SAED characterization. W.P., H.W., J.L., G.N. and J.T. wrote the paper. All authors commented on the manuscript.

Corresponding authors

Correspondence to Guangda Niu, Qingguo Xie or Jiang Tang.

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Pan, W., Wu, H., Luo, J. et al. Cs2AgBiBr6 single-crystal X-ray detectors with a low detection limit. Nature Photon 11, 726–732 (2017). https://doi.org/10.1038/s41566-017-0012-4

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