Amine-Salt-Assisted Solution Crystallization of Inorganic Perovskite Single Crystals for High-Performance X-Ray Detection
Corresponding Author: Shengzhong Frank Liu
Nano-Micro Letters,
Vol. 18 (2026), Article Number: 421
Abstract
Inorganic perovskite CsPbCl3 single crystals (SCs) are promising for stable and high-performance X-ray detection due to their high X-ray absorption, superior optoelectronic properties, and superior chemical and thermal stability. However, the size of CsPbCl3 SCs grown via low-energy-consumption solution methods remains limited to below 1 mm, primarily because of the limited solubility of raw materials in solvents and the lack of effective growth techniques. In this work, an amine-salt-assisted solution crystallization strategy is developed to grow high-quality CsPbCl3 SCs with size up to 15 mm. This significant size improvement is enabled by a 13-fold increase in precursor solubility, achieved by constructing hydrogen bond interactions between the amine salt and insoluble raw materials. Consequently, the SCs exhibit high μτ product (6.3 × 10–3 cm2 V−1), low trap density (2.9 × 1010 cm−3), and large resistivity (1.7 × 109 Ω cm). Therefore, the SC detectors achieve a record-high sensitivity of 76,624 μC Gy−1 cm−2 and a low detection limit of 47.9 nGy s−1 even under low bias voltages, enabling high contrast X-ray imaging. This ingenious and executable low-temperature solution crystallization strategy combined with superior X-ray detection performance makes CsPbCl3 SCs promising to advance the low-cost development of safe radiation detection systems.
Highlights:
1 An amine-salt-assisted solution crystallization strategy is developed to grow high-quality CsPbCl3 single crystals (SCs) with a size as large as 15 mm, the SCs exhibit a high carrier mobility-lifetime product, low trap density, and large resistivity.
2 The CsPbCl3 SC X-ray detector achieved a high detection sensitivity of 76,624 μC Gy-1 cm-2 and a low detection limit of 47.9 nGy s-1, a short response time of 700 μs, therefore realized high contrast X-ray imaging.
Keywords
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References
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D. Chu, N. Liu, S. Xie, Y. Li, J. Chen et al., Stable and ultrasensitive X-ray detectors based on oriented single-crystal perovskite rods. Adv. Mater. 37(27), 2500101 (2025). https://doi.org/10.1002/adma.202500101
D. Chu, B. Jia, N. Liu, Y. Zhang, X. Li et al., Lattice engineering for stabilized black FAPbI3 perovskite single crystals for high-resolution X-ray imaging at the lowest dose. Sci. Adv. 9(35), eadh2255 (2023). https://doi.org/10.1126/sciadv.adh2255
J. Yu, Y. Luo, N. Tian, Y. Liu, Z. Yang et al., Large scale lead-free perovskite polycrystalline wafer achieved by hot-pressed strategy for high-performance X-ray detection. Adv. Mater. 37(4), 2413709 (2025). https://doi.org/10.1002/adma.202413709
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J. Yan, Q. Zheng, S.-P. Wang, Y.-Z. Tian, W.-Q. Gong et al., Multifunctional organic–inorganic hybrid perovskite microcrystalline engineering and electromagnetic response switching multi-band devices. Adv. Mater. 35(25), 2300015 (2023). https://doi.org/10.1002/adma.202300015
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M. Girolami, F. Matteocci, S. Pettinato, V. Serpente, E. Bolli et al., Metal-halide perovskite submicrometer-thick films for ultra-stable self-powered direct X-ray detectors. Nano-Micro Lett. 16(1), 182 (2024). https://doi.org/10.1007/s40820-024-01393-6
D.B. Straus, S. Guo, R.J. Cava, Kinetically stable single crystals of perovskite-phase CsPbI3. J. Am. Chem. Soc. 141(29), 11435–11439 (2019). https://doi.org/10.1021/jacs.9b06055
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L. Pan, Z. Liu, C. Welton, V.V. Klepov, J.A. Peters et al., Ultrahigh-flux X-ray detection by a solution-grown perovskite CsPbBr3 single-crystal semiconductor detector. Adv. Mater. 35(25), 2211840 (2023). https://doi.org/10.1002/adma.202211840
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Y. He, C.C. Stoumpos, I. Hadar, Z. Luo, K.M. McCall et al., Demonstration of energy-resolved γ-Ray detection at room temperature by the CsPbCl3 perovskite semiconductor. J. Am. Chem. Soc. 143(4), 2068–2077 (2021). https://doi.org/10.1021/jacs.0c12254
W. Xu, J. Liu, B. Dong, J. Huang, H. Shi et al., Atomic-scale imaging of ytterbium ions in lead halide perovskites. Sci. Adv. 9(35), eadi7931 (2023). https://doi.org/10.1126/sciadv.adi7931
X. Li, C. Liu, F. Ding, Z. Lu, P. Gao et al., Ultra-stable and sensitive ultraviolet photodetectors based on monocrystalline perovskite thin films. Adv. Funct. Mater. 33(15), 2213360 (2023). https://doi.org/10.1002/adfm.202213360
M. Gong, M. Alamri, D. Ewing, S.M. Sadeghi, J.Z. Wu, Localized surface plasmon resonance enhanced light absorption in AuCu/CsPbCl3 core/shell nanocrystals. Adv. Mater. 32(26), 2002163 (2020). https://doi.org/10.1002/adma.202002163
P. Gui, H. Zhou, F. Yao, Z. Song, B. Li et al., High-performance X-ray detection based on perovskite materials with enhanced stability. Small 15(39), 1902618 (2019). https://doi.org/10.1002/smll.201902618
S.G. Ji, I.J. Park, H. Chang, J.H. Park, G.P. Hong et al., Stable pure-iodide wide-band-gap perovskites for efficient Si tandem cells via kinetically controlled phase evolution. Joule 6(10), 2390–2405 (2022). https://doi.org/10.1016/j.joule.2022.08.006
N. Pellet, J. Teuscher, J. Maier, M. Grätzel, Transforming hybrid organic inorganic perovskites by rapid halide exchange. Chem. Mater. 27(6), 2181–2188 (2015). https://doi.org/10.1021/acs.chemmater.5b00281
Q.A. Akkerman, V. D’Innocenzo, S. Accornero, A. Scarpellini, A. Petrozza et al., Tuning the optical properties of cesium lead halide perovskite nanocrystals by anion exchange reactions. J. Am. Chem. Soc. 137(32), 10276–10281 (2015). https://doi.org/10.1021/jacs.5b05602
N. Livakas, S. Toso, Y.P. Ivanov, T. Das, S. Chakraborty et al., CsPbCl3 → CsPbI3 exchange in perovskite nanocrystals proceeds through a jump-the-gap reaction mechanism. J. Am. Chem. Soc. 145(37), 20442–20450 (2023). https://doi.org/10.1021/jacs.3c06214
Y. Zhang, J. Hao, Z. Zhao, J. Pi, R. Shi et al., Lead-free perovskite single crystal linear array detector for high-resolution X-ray imaging. Adv. Mater. 36(24), e2310831 (2024). https://doi.org/10.1002/adma.202310831
Y. Liu, Y. Zhang, X. Zhu, Z. Yang, W. Ke et al., Inch-sized high-quality perovskite single crystals by suppressing phase segregation for light-powered integrated circuits. Sci. Adv. 7(7), eabc8844 (2021). https://doi.org/10.1126/sciadv.abc8844
Y. Liu, Y. Zhang, X. Zhu, J. Feng, I. Spanopoulos et al., Triple-cation and mixed-halide perovskite single crystal for high-performance X-ray imaging. Adv. Mater. 33(8), e2006010 (2021). https://doi.org/10.1002/adma.202006010
L. Zhao, Y. Zhou, Z. Shi, Z. Ni, M. Wang et al., High-yield growth of FACsPbBr3 single crystals with low defect density from mixed solvents for gamma-ray spectroscopy. Nat. Photon. 17, 315–323 (2023). https://doi.org/10.1038/s41566-023-01154-8
M. Li, S. Wang, A. Wood, J.D. Yeager, S.P. Stepanoff et al., Defect repairing in lead bromide perovskite single crystals with biasing and bromine for X-ray photon-counting detectors. Nat. Mater. 24(12), 1993–2000 (2025). https://doi.org/10.1038/s41563-025-02310-x
J. Pang, H. Wu, H. Li, T. Jin, J. Tang et al., Reconfigurable perovskite X-ray detector for intelligent imaging. Nat. Commun. 15(1), 1769 (2024). https://doi.org/10.1038/s41467-024-46184-0
R. Shi, J. Pi, D. Chu, B. Jia, Z. Zhao et al., Promoting band splitting through symmetry breaking in inorganic halide perovskite single crystals for high-sensitivity X-ray detection. ACS Energy Lett. 8(11), 4836–4847 (2023). https://doi.org/10.1021/acsenergylett.3c01661
X. Pan, T. An, J. Sun, H. Dong, Z. Ma et al., Thermodynamically induced crystal restructuring to make CsPbCl3 single crystal films for weak light detection. Nano Res. 17(11), 9775–9783 (2024). https://doi.org/10.1007/s12274-024-6967-9
X. Zhang, D. Chu, B. Jia, Z. Zhao, J. Pi et al., Heterointerface design of perovskite single crystals for high-performance X-ray imaging. Adv. Mater. 36(3), e2305513 (2024). https://doi.org/10.1002/adma.202305513
S. Yang, S. Chen, E. Mosconi, Y. Fang, X. Xiao et al., Stabilizing halide perovskite surfaces for solar cell operation with wide-bandgap lead oxysalts. Science 365(6452), 473–478 (2019). https://doi.org/10.1126/science.aax3294
M. Chen, X. Dong, D. Chu, B. Jia, X. Zhang et al., Interlayer-spacing engineering of lead-free perovskite single crystal for high-performance X-ray imaging. Adv. Mater. 35(18), 2211977 (2023). https://doi.org/10.1002/adma.202211977
D. Liu, Y. Zheng, X.Y. Sui, X.F. Wu, C. Zou et al., Universal growth of perovskite thin monocrystals from high solute flux for sensitive self-driven X-ray detection. Nat. Commun. 15(1), 2390 (2024). https://doi.org/10.1038/s41467-024-46712-y
N. Liu, D. Chu, X. Xin, J. Tian, Y. Jiang et al., Unveiling the role of cesium in halide perovskite single crystal for stable and ultrasensitive X-ray detection. Adv. Funct. Mater. 36(21), 2504203 (2026). https://doi.org/10.1002/adfm.202504203
Y. Fang, J. Huang, Resolving weak light of sub-picowatt per square centimeter by hybrid perovskite photodetectors enabled by noise reduction. Adv. Mater. 27(17), 2804–2810 (2015). https://doi.org/10.1002/adma.201500099
Y. Liang, Z. Zhao, J. Hao, Y. Zhang, D. Chu et al., Interlamellar-spacing engineering of stable and toxicity-reduced 2D perovskite single crystal for high-resolution X-ray imaging. Nano Lett. 24(27), 8436–8444 (2024). https://doi.org/10.1021/acs.nanolett.4c02507