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Extreme γ-ray radiation hardness and high scintillation yield in perovskite nanocrystals

Nature Photonics volume 16, pages 860–868 (2022)Cite this article

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Abstract

Radiation detection is of utmost importance in fundamental scientific research, as well as medical diagnostics, homeland security, environmental monitoring and industrial control. Lead halide perovskites (LHPs) are attracting growing attention as high-atomic-number materials for next-generation scintillators and photoconductors for ionizing radiation detection. To unlock their full potential as reliable and cost-effective alternatives to conventional materials, it is necessary for LHPs to conjugate high scintillation yields with emission stability under high doses of ionizing radiation. To date, no definitive solution has been devised to optimize the scintillation efficiency and kinetics of LHPs and nothing is known of their radiation hardness for doses above a few kilograys, to the best of our knowledge. Here we demonstrate that CsPbBr3 nanocrystals exhibit exceptional radiation hardness for γ-radiation doses as high as 1 MGy. Spectroscopic and radiometric experiments highlight that despite their defect tolerance, standard CsPbBr3 nanocrystals suffer from electron trapping in dense surface defects that are eliminated by post-synthesis fluorination. This results in >500% enhancement in scintillation efficiency, which becomes comparable to commercial scintillators, and still retaining exceptional levels of radiation hardness. These results have important implications for the widespread use of LHPs in ultrastable and efficient radiation detectors.

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Fig. 1: Structural and spectroscopic properties of untreated and fluoride-treated CsPbBr3 NCs.
Fig. 2: Extreme radiation hardness experiments.
Fig. 3: Thermal liberation of electrons from shallow defect states.
Fig. 4: Long-lived non-radiative traps and detrapping processes.

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The data that support the findings of this study are available from the corresponding authors upon reasonable request.

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Acknowledgements

This work received funding from the European Union’s Horizon 2020 Research and Innovation programme under grant agreement no. 101004761 (AIDAINNOVA) and financial support from Guangdong Province’s 2018–2019 Key R&D Program (2019B010924001) and the National Natural Science Foundation of China (NSFC 22175113). We thank R. Huang from East China Normal University for help with the aberration-corrected scanning transmission electron microscopy measurements and analyses.

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Author notes

  1. These authors contributed equally: Matteo L. Zaffalon, Francesca Cova.

Authors and Affiliations

  1. Dipartimento di Scienza dei Materiali, Università degli Studi Milano-Bicocca, Milan, Italy

    Matteo L. Zaffalon, Francesca Cova, Francesco Carulli, Andrea Erroi, Carmelita Rodà, Jacopo Perego, Angiolina Comotti, Mauro Fasoli, Francesco Meinardi, Anna Vedda & Sergio Brovelli

  2. Istituto Nazionale di Fisica Nucleare (INFN), Sezione di Milano-Bicocca, Milan, Italy

    Francesca Cova, Mauro Fasoli, Anna Vedda & Sergio Brovelli

  3. School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai, China

    Mingming Liu

  4. ENEA Fusion and Technology for Nuclear Safety and Security Department, Casaccia R.C., Rome, Italy

    Alessia Cemmi & Ilaria Di Sarcina

  5. IMEM-CNR Institute, Parma, Italy

    Francesca Rossi

  6. Macao Institute of Materials Science and Engineering (MIMSE), Macau University of Science and Technology, Macao, China

    Liang Li

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  1. Matteo L. Zaffalon
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Contributions

S.B. conceived this study. M.L. synthesized and characterized the NCs under the supervision of L.L. A. Cemmi and I.D.S. performed the irradiation procedures. J.P. performed the XRD characterization under the supervision of A. Comotti M.L.Z. performed the optical experiments under the supervision of F.M. and S.B. F. Cova performed the radiometric characterization under the supervision of M.F. and A.V. F.R. performed the CL experiments. M.L.Z., F. Cova, F. Carulli, C.R., A.E. and S.B. analysed the data. S.B. wrote the paper in consultation with all the authors. M.L.Z. and F. Cova contributed equally to this work.

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Correspondence to Liang Li, Anna Vedda or Sergio Brovelli.

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Zaffalon, M.L., Cova, F., Liu, M. et al. Extreme γ-ray radiation hardness and high scintillation yield in perovskite nanocrystals. Nat. Photon. 16, 860–868 (2022). https://doi.org/10.1038/s41566-022-01103-x

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