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High-yield growth of FACsPbBr3 single crystals with low defect density from mixed solvents for gamma-ray spectroscopy

Nature Photonics volume 17, pages 315–323 (2023)Cite this article

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Abstract

Metal halide perovskites are promising candidates for room-temperature gamma-ray spectrum detectors; however, it is hard to grow high-quality single crystals that are performance competitive with existing materials. Here we report the growth of centimetre-sized formamidinium-caesium lead bromide (FACsPbBr3) single crystals at high yield from low-purity (98%) precursors using a solution method. The introduction of formamidinium into CsPbBr3 reduces defect density in crystals by eliminating the phase transition upon cooling from growth temperature to room temperature. A mixed solvent is applied to match the solubility slopes of CsPbBr3 and FAPbBr3, resulting in successful incorporation of caesium into FAPbBr3 at FA:Cs ratios from 0 to 1. As-grown FACsPbBr3 exhibits a high resistivity of 9.5 × 109 Ω cm, balanced hole and electron mobility-lifetime products of (2.2–3.2) × 10−3 cm2 V−1, and a record low deep trap density of 5.6 × 1010 cm−3, yielding a high charge collection efficiency of 84% under gamma-rays. FACsPbBr3 spectrum detectors achieve an energy resolution of 2.9% for 662 keV 137Cs γ-rays. Over 65% of the FACsPbBr3 crystals exhibit good γ-ray spectral performance. FACsPbBr3 single crystals show excellent stability under large biases of up to 1,000 V and no degradation of spectrum performance after seven months.

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Fig. 1: Phase transition and growth of FAxCs1–xPbBr3 single crystals.
Fig. 2: Crystal structure and bandgap of FAxCs1–xPbBr3 crystals.
Fig. 3: FAxCs1–xPbBr3 crystal quality evaluation.
Fig. 4: Spectral response of FA0.9Cs0.1PbBr3 detectors to different γ-ray sources.
Fig. 5: Optoelectronic properties of FACsPbBr3 crystals.

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The authors declare that all relevant data supporting the findings of this study are available within the paper and its Supplementary Information.

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Acknowledgements

This work is financially supported in part by University of North Carolina at Chapel Hill and the Defense Threat Reduction Agency under award no. HDTRA1-20-2-0002. We thank P. Sellin at the University of Surrey for insightful discussions. This crystal characterization was supported in part by the Center for Hybrid Organic Inorganic Semiconductors for Energy (CHOISE), an Energy Frontier Research Center funded by the Office of Basic Energy Sciences, Office of Science within the US Department of Energy (DOE). The views expressed in the article do not necessarily represent the views of the DOE or the US Government.

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Authors and Affiliations

  1. Department of Applied Physical Sciences, University of North Carolina at Chapel Hill, Chapel Hill, NC, USA

    Liang Zhao, Ying Zhou, Zhifang Shi, Zhenyi Ni, Mengru Wang, Ye Liu & Jinsong Huang

  2. Perotech Inc, Chapel Hill, NC, USA

    Ye Liu

  3. Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, NC, USA

    Jinsong Huang

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Contributions

J.H. conceived and supervised the project. L.Z. and Y.L. synthesized the crystals. L.Z. fabricated the devices, and measured the electronic properties and γ-ray spectral performances. Y.Z. built up γ-ray testing system, and measured PL and TRPL. Z.S. contributed to the XRD analysis. Z.N. performed DLCP measurements. M.W. performed EDX measurements.

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Correspondence to Jinsong Huang.

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Supplementary Figs. 1–19 and Tables 1–9.

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Zhao, L., Zhou, Y., Shi, Z. 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

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