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Title: Zero-dimensional Cs 4EuX 6 (X = Br, I) all-inorganic perovskite single crystals for gamma-ray spectroscopy

Abstract

Organic–inorganic and all-inorganic halide perovskites have become leading candidates toward high-performance optoelectronic devices and radiation detectors. In this work, we report novel zero-dimensional Cs 4EuX 6 (X = Br, I) perovskite single crystals as self-activated scintillators with superior performance for gamma-ray spectroscopy. Both Cs 4EuBr 6 and Cs 4EuI 6 single crystals grown by the Bridgman method were determined to have the trigonal crystal structure with the R$$\bar{3}$$c space group, and have a melting point of approximately 540°C. Cs 4EuBr 6 and Cs4EuI 6 exhibit blue emission under UV excitation and high light yields of 78,000 ± 4000 photons/MeV and 53,000 ± 3000 photons/MeV under 137Cs gamma-ray irradiation, respectively. In particular, the former represents the best result achieved for self-activated scintillators thus far. Thermally stimulated luminescence studies and density functional theory calculations elucidate the correlation between halogen vacancies and long-lived emission (afterglow) at room temperature in Cs4EuX 6 (X=Br, I) single crystals. In conclusion, our findings not only demonstrate the high gamma-ray detection efficiency in Cs 4EuX 6 (X=Br, I), but will further promote the development of 0D metal halide-based novel luminescent and radiation detection materials.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [5]; ORCiD logo [6];  [1];  [1];  [1];  [7];  [8];  [9]
  1. Univ. of Tennessee, Knoxville, TN (United States). Scintillation Materials Research Center; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Materials Science and Engineering
  2. East China Normal Univ. (ECNU), Shanghai (China). Key Lab. of Polar Materials and Devices (Ministry of Education); East China Normal Univ. (ECNU), Shanghai (China). Dept. of Physics; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division
  4. Beihang Univ., Beijing (China). Key Lab. of Micro-Nano Measurement-Manipulation and Physics (Ministry of Education), Dept. of Physics
  5. East China Normal Univ. (ECNU), Shanghai (China). Key Lab. of Polar Materials and Devices (Ministry of Education)
  6. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
  7. Univ. of Tennessee, Knoxville, TN (United States). Scintillation Materials Research Center; Univ. of Tennessee, Knoxville, TN (United States). Bredesen Center for Interdisciplinary Research and Graduate Education
  8. Univ. of Tennessee, Knoxville, TN (United States). Scintillation Materials Research Center
  9. Univ. of Tennessee, Knoxville, TN (United States). Scintillation Materials Research Center; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Materials Science and Engineering; Univ. of Tennessee, Knoxville, TN (United States). Bredesen Center for Interdisciplinary Research and Graduate Education; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Nuclear Engineering
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1459274
Alternate Identifier(s):
OSTI ID: 1455088
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry C
Additional Journal Information:
Journal Volume: 6; Journal Issue: 25; Journal ID: ISSN 2050-7526
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Perovskites; zero-dimensional; radiation detection; scintillators

Citation Formats

Wu, Yuntao, Han, Dan, Chakoumakos, Bryan C., Shi, Hongliang, Chen, Shiyou, Du, Mao-Hua, Greeley, Ian, Loyd, Matthew, Rutstrom, Daniel J., Stand, Luis, Koschan, Merry, and Melcher, Charles L. Zero-dimensional Cs4EuX6 (X = Br, I) all-inorganic perovskite single crystals for gamma-ray spectroscopy. United States: N. p., 2018. Web. doi:10.1039/C8TC01458B.
Wu, Yuntao, Han, Dan, Chakoumakos, Bryan C., Shi, Hongliang, Chen, Shiyou, Du, Mao-Hua, Greeley, Ian, Loyd, Matthew, Rutstrom, Daniel J., Stand, Luis, Koschan, Merry, & Melcher, Charles L. Zero-dimensional Cs4EuX6 (X = Br, I) all-inorganic perovskite single crystals for gamma-ray spectroscopy. United States. doi:10.1039/C8TC01458B.
Wu, Yuntao, Han, Dan, Chakoumakos, Bryan C., Shi, Hongliang, Chen, Shiyou, Du, Mao-Hua, Greeley, Ian, Loyd, Matthew, Rutstrom, Daniel J., Stand, Luis, Koschan, Merry, and Melcher, Charles L. Fri . "Zero-dimensional Cs4EuX6 (X = Br, I) all-inorganic perovskite single crystals for gamma-ray spectroscopy". United States. doi:10.1039/C8TC01458B. https://www.osti.gov/servlets/purl/1459274.
@article{osti_1459274,
title = {Zero-dimensional Cs4EuX6 (X = Br, I) all-inorganic perovskite single crystals for gamma-ray spectroscopy},
author = {Wu, Yuntao and Han, Dan and Chakoumakos, Bryan C. and Shi, Hongliang and Chen, Shiyou and Du, Mao-Hua and Greeley, Ian and Loyd, Matthew and Rutstrom, Daniel J. and Stand, Luis and Koschan, Merry and Melcher, Charles L.},
abstractNote = {Organic–inorganic and all-inorganic halide perovskites have become leading candidates toward high-performance optoelectronic devices and radiation detectors. In this work, we report novel zero-dimensional Cs4EuX6 (X = Br, I) perovskite single crystals as self-activated scintillators with superior performance for gamma-ray spectroscopy. Both Cs4EuBr6 and Cs4EuI6 single crystals grown by the Bridgman method were determined to have the trigonal crystal structure with the R$\bar{3}$c space group, and have a melting point of approximately 540°C. Cs4EuBr6 and Cs4EuI6 exhibit blue emission under UV excitation and high light yields of 78,000 ± 4000 photons/MeV and 53,000 ± 3000 photons/MeV under 137Cs gamma-ray irradiation, respectively. In particular, the former represents the best result achieved for self-activated scintillators thus far. Thermally stimulated luminescence studies and density functional theory calculations elucidate the correlation between halogen vacancies and long-lived emission (afterglow) at room temperature in Cs4EuX6 (X=Br, I) single crystals. In conclusion, our findings not only demonstrate the high gamma-ray detection efficiency in Cs4EuX6 (X=Br, I), but will further promote the development of 0D metal halide-based novel luminescent and radiation detection materials.},
doi = {10.1039/C8TC01458B},
journal = {Journal of Materials Chemistry C},
number = 25,
volume = 6,
place = {United States},
year = {2018},
month = {6}
}

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Cited by: 5 works
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Figures / Tables:

Figure 1 Figure 1: (a) A 12-mm diameter as-grown Cs4EuBr6 single crystal. (b) A 7-mm diameter as-grown Cs4EuI6 single crystal and (c) a 1-mm thick Cs4EuI6 slab. (d) Optical transmission spectra of 1 mm thick Cs4EuBr6 and Cs4EuI6 crystal slabs. (e) Differential scanning calorimeter curves of Cs4EuBr6 and Cs4EuI6 single crystals. (f)more » DVS curves of Cs4EuBr6 and Cs4EuI6 single crystals. The DVS curve of a NaI standard sample is also shown for comparison.« less

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    journal, July 2014


    Low trap-state density and long carrier diffusion in organolead trihalide perovskite single crystals
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    Electron-hole diffusion lengths > 175 μm in solution-grown CH 3 NH 3 PbI 3 single crystals
    journal, January 2015


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    • Du, Mao-Hua
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    • DOI: 10.1149/2.0011601jss

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