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Suppressed ion migration for high-performance X-ray detectors based on atmosphere-controlled EFG-grown perovskite CsPbBr3 single crystals

Nature Photonics volume 18, pages 870–877 (2024)Cite this article

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Abstract

Halide perovskites have shown great potential for X-ray detection in medical imaging and product inspection applications. However, the ion migration in perovskites causes large noise and baseline drift, deteriorating the X-ray detection and imaging performance. Here we adopt the atmosphere-controlled edge-defined film-fed growth (EFG) method to grow high-quality shape-controlled CsPbBr3 single crystals (SCs) in an Ar and HBr mixed atmosphere. Compared with the vertical Bridgman (VB)-CsPbBr3 SCs, the EFG-CsPbBr3 SCs show a much lower trap density, a higher resistivity (1.61 × 1010 Ω cm) and a larger ion migration activation energy (0.378 eV), decreasing the leakage current and baseline drift. An X-ray detector based on EFG-CsPbBr3 SCs hence exhibits outstanding balanced performance, with a negligible dark-current drift of 1.68 × 10−9 μA cm−1 s−1 V−1, an incredibly low detection limit of 10.81 nGyair s−1 and a sensitivity of 46,180 μC Gyair−1 cm−2 under a high electric field of 5,000 V cm−1. Furthermore, the detector maintains a stable response for 30 days. Our work provides an effective strategy to improve lead-halide perovskite SCs for high-performance X-ray detection and imaging.

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Fig. 1: Growth of CsPbBr3 SCs by the EFG method.
Fig. 2: Comparison of the photoelectric properties of EFG-CsPbBr3 and VB-CsPbBr3.
Fig. 3: Ion migration properties of EFG-CsPbBr3 and VB-CsPbBr3.
Fig. 4: X-ray detection responses and sensitivity.
Fig. 5: X-ray detection limits and imaging.

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Data availability

The data that support the findings of this study are available within the paper. Additional data are available from the corresponding authors upon request. Source data are provided with this paper.

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Acknowledgements

This work was supported financially by the National Key Research and Development Program of China (grant nos. 2022YFB3204101 and 2023YFB3507900), the National Natural Science Foundation of China (grant nos. 62274103, 51972194 and 51932004) and the 111 Project 2.0 (grant no. BP2018013).

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Authors and Affiliations

  1. State Key Laboratory of Crystal Materials, Institute of Crystal Materials, Shandong University, Jinan, China

    Yunqiu Hua, Guodong Zhang, Xue Sun, Peng Zhang, Xiang Li, Zhongjun Zhai, Fucai Cui, Hongjie Liu, Jiaxin Liu & Xutang Tao

  2. State Key Laboratory of Solidification Processing, School of Materials Science and Engineering, Northwestern Polytechnical University, Xi’an, China

    Yingying Hao & Yadong Xu

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

    Yujie Yang & Qianqian Lin

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  1. Yunqiu Hua
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Contributions

G.Z. and X.T. conceived and supervised the project. Y. Hua and G.Z. synthesized, characterized and grew the single crystals. Y. Hua and Z.Z. fabricated the devices and characterized the detector performance. X.S. and X.L. sputtered the electrodes. Y. Hao and Y.X. performed the ToF measurements. Y.Y. and Q.L. performed the TRMC measurement. Y. Hua and P.Z. performed the impedance spectroscopy measurement. X.L. and F.C. performed theoretical simulations and analysed the results. J.L. and H.L. assisted with device optimization and data analysis. Y. Hua, G.Z. and X.T. wrote the paper. All authors discussed the results and commented on the paper.

Corresponding authors

Correspondence to Guodong Zhang or Xutang Tao.

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Supplementary information

Supplementary Information

Supplementary Figs. 1–43, Discussion and Tables 1–9.

Supplementary Video 1

Real-time evolution of the EFG growth at different stages for the cylindrical CsPbBr3 crystal.

Source data

Source Data Fig. 2

Comparison of the photoelectric properties of EFG-CsPbBr3 and VB-CsPbBr3.

Source Data Fig. 3

Ion migration properties of EFG-CsPbBr3 and VB-CsPbBr3.

Source Data Fig. 4

X-ray detection responses and sensitivity.

Source Data Fig. 5

X-ray detection limits and imaging.

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Hua, Y., Zhang, G., Sun, X. et al. Suppressed ion migration for high-performance X-ray detectors based on atmosphere-controlled EFG-grown perovskite CsPbBr3 single crystals. Nat. Photon. 18, 870–877 (2024). https://doi.org/10.1038/s41566-024-01480-5

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