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Growth of High-Purity CsPbBr3 Crystals for Enhanced Gamma-Ray Detection
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    Growth of High-Purity CsPbBr3 Crystals for Enhanced Gamma-Ray Detection
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    • Duck Young Chung
      Duck Young Chung
      Materials Science Division, Argonne National Laboratory, Argonne, Illinois 60439, United States
    • Wenwen Lin
      Wenwen Lin
      Materials Science Division, Argonne National Laboratory, Argonne, Illinois 60439, United States
      Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States
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    • Mustafa Unal
      Mustafa Unal
      Materials Science Division, Argonne National Laboratory, Argonne, Illinois 60439, United States
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    • Quoc Vuong Phan
      Quoc Vuong Phan
      Materials Science Division, Argonne National Laboratory, Argonne, Illinois 60439, United States
      Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States
    • Indra R. Pandey
      Indra R. Pandey
      Materials Science Division, Argonne National Laboratory, Argonne, Illinois 60439, United States
      Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States
    • Richard Vitt
      Richard Vitt
      Materials Science Division, Argonne National Laboratory, Argonne, Illinois 60439, United States
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    • Yihui He
      Yihui He
      Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States
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    • Mercouri G. Kanatzidis*
      Mercouri G. Kanatzidis
      Materials Science Division, Argonne National Laboratory, Argonne, Illinois 60439, United States
      Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States
      *Email: [email protected]
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    Crystal Growth & Design

    Cite this: Cryst. Growth Des. 2024, 24, 22, 9590–9600
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    https://doi.org/10.1021/acs.cgd.4c01109
    Published November 5, 2024
    Copyright © 2024 American Chemical Society

    Abstract

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    High-quality CsPbBr3 crystals hold significant potential for gamma-ray detection due to their remarkable optoelectronic properties. This study details an optimized production process using the Bridgman method to achieve highly pure CsPbBr3 crystals. By implementing rigorous synthesis and purification techniques, we successfully reduced the total impurity levels to 9 ppm, as confirmed by glow discharge mass spectroscopy (GDMS). The resulting CsPbBr3 crystals demonstrate exceptional performance, including high transparency, intense photoemission, and prolonged photoluminescence decay times. These properties facilitate superior gamma-ray detection with an energy resolution of 1.4% for the 137Cs 662 keV gamma-rays, comparable to commercial Cd1–xZnxTe (CZT) detectors. Our findings underscore the critical relationship between material purity and detector performance, highlighting the potential of CsPbBr3 as a cost-effective alternative in radiation detection applications. Further studies on defect origins and electronic states are necessary to fully leverage the capabilities of CsPbBr3 crystals in practical high-energy radiation detection systems.

    Copyright © 2024 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.cgd.4c01109.

    • Temperature profile applied to the crystal growth process using the Bridgman method, and the temperature gradient near the crystallization point is approximately 17.5 °C/cm (Figure S1); (a) CsPbBr3 powder synthesized in aqueous HBr (48%) solution and (b) crystal boule grown using the material (Figure S2); (a) CsPbBr3 crystals grown in the DMSO/cyclohexanol solution, and then (b) dried at 400 °C, and (c) melted at 600 °C and (d) crystal purity after multiple Bridgman processes at a growth rate of 2 mm/h to purify the CsPbBr3 prepared in DMSO (Figure S3); X-ray diffraction patterns of (a) pure CsPbBr3 and (b) white decomposition product CsPb2Br5 resulting from the treatment of CsPbBr3 in water compared with the calculated patterns (black) using the crystal structure data (Figure S4); photoluminescence spectra of two low-quality crystals that exhibit additional peaks near 500 and 560 nm and a broad emission in the range of 550–800 nm owing to the secondary phase and defects and crystals (I) and (II) grown under PbBr2 and CsBr-rich conditions, respectively (Figure S5); GDMS analysis for the crystals grown using (a) unpurified and (b) purified CsPbBr3 and (c) crystals of the impure end after zone refining (Table S1) (PDF)

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    Crystal Growth & Design

    Cite this: Cryst. Growth Des. 2024, 24, 22, 9590–9600
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.cgd.4c01109
    Published November 5, 2024
    Copyright © 2024 American Chemical Society

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