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Dopant compensation in alloyed CH3NH3PbBr3−xClx perovskite single crystals for gamma-ray spectroscopy

Nature Materials volume 16, pages 826–833 (2017)Cite this article

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Abstract

Organic–inorganic halide perovskites (OIHPs) bring an unprecedented opportunity for radiation detection with their defect-tolerance nature, large mobility–lifetime product, and simple crystal growth from solution. Here we report a dopant compensation in alloyed OIHP single crystals to overcome limitations of device noise and charge collection, enabling γ-ray spectrum collection at room temperature. CH3NH3PbBr3 and CH3NH3PbCl3 are found to be p-type and n-type doped, respectively, whereas dopant-compensated CH3NH3PbBr2.94Cl0.06 alloy has over tenfold improved bulk resistivity of 3.6 × 109 Ω cm. Alloying also increases the hole mobility to 560 cm2 V−1 s−1, yielding a high mobility–lifetime product of 1.8 × 10−2 cm2 V−1. The use of a guard ring electrode in the detector reduces the crystal surface leakage current and device dark current. A distinguishable 137Cs energy spectrum with comparable or better resolution than standard scintillator detectors is collected under a small electric field of 1.8 V mm−1 at room temperature.

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Figure 1: Cl− alloying for dopant compensation.
Figure 2: Cl− alloying to suppress dark current.
Figure 3: Mobility and μτ product improvement.
Figure 4: Photodetector performance.
Figure 5: γ-ray detector performance.

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Acknowledgements

This work is financially supported by the Defense Threat Reduction Agency (Award No. HDTRA1-14-1-0030). We thank Y. Yan at the University of Toledo for the discussion of the doping mechanism in the mixed-halide perovskites.

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Author notes

  1. Haotong Wei and Dylan DeSantis: These authors contributed equally to this work.

Authors and Affiliations

  1. Department of Mechanical and Materials Engineering, University of Nebraska-Lincoln, Lincoln, Nebraska, 68588, USA

    Haotong Wei, Wei Wei, Yehao Deng & Jinsong Huang

  2. Department of Mechanical and Aerospace Engineering, Nuclear Engineering Program, Ohio State University, Columbus, Ohio, 43210, USA

    Dylan DeSantis & Lei Cao

  3. Department of Chemical Engineering, Optoelectronic Materials Section, Delft University of Technology, 2628 BL Delft, The Netherlands

    Dengyang Guo & Tom J. Savenije

  4. Department of Applied Physical Sciences, University of North Carolina, Chapel Hill, North Carolina, 27599, USA

    Jinsong Huang

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Contributions

J.H. conceived and supervised the project. H.W. synthesized crystals, fabricated the devices, and measured the optoelectronic properties and X-ray detector sensitivity. D.D. performed and L.C. supervised the 137Cs energy spectrum measurement. H.W. and W.W. calibrated the X-ray dose rate. Y.D. carried out the XRD measurement. D.G. and T.J.S. contributed the charge carrier lifetime measurement. J.H., H.W., D.D. and L.C. wrote the manuscript, and all the authors reviewed the manuscript.

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Correspondence to Jinsong Huang.

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The authors declare no competing financial interests.

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Wei, H., DeSantis, D., Wei, W. et al. Dopant compensation in alloyed CH3NH3PbBr3−xClx perovskite single crystals for gamma-ray spectroscopy. Nature Mater 16, 826–833 (2017). https://doi.org/10.1038/nmat4927

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