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Title: Identification and Suppression of Point Defects in Bromide Perovskite Single Crystals Enabling Gamma‐Ray Spectroscopy

Journal Article · · Advanced Materials
ORCiD logo [1];  [1];  [1];  [2];  [3];  [4];  [4];  [5];  [5];  [2]; ORCiD logo [6]
  1. Department of Applied Physical Sciences University of North Carolina Chapel Hill NC 27599 USA
  2. Physics SUPA School of Science and Engineering University of Dundee Dundee DD1 4HN UK
  3. Department of Physics Chalmers University of Technology Gothenburg SE‐41296 Sweden
  4. Institute of Radiation Physics Helmholtz‐Zentrum Dresden‐Rossendorf Bautzner Landstraße 400 01328 Dresden Germany
  5. Chemistry and Nanoscience Center National Renewable Energy Laboratory Golden CO 80401 USA
  6. Department of Applied Physical Sciences University of North Carolina Chapel Hill NC 27599 USA, Department of Chemistry University of North Carolina Chapel Hill NC 27599 United States

Abstract Methylammonium lead tribromide (MAPbBr 3 ) stands out as the most easily grown wide‐band‐gap metal halide perovskite. It is a promising semiconductor for room‐temperature gamma‐ray ( γ ‐ray) spectroscopic detectors, but no operational devices are realized. This can be largely attributed to a lack of understanding of point defects and their influence on detector performance. Here, through a combination of crystal growth design and defect characterization, including positron annihilation and impedance spectroscopy, the presence of specific point defects are identified and correlated to detector performance. Methylammonium (MA) vacancies, MA interstitials, and Pb vacancies are identified as the dominant charge‐trapping defects in MAPbBr 3 crystals, while Br vacancies caused doping. The addition of excess MABr reduces the MA and Br defects and so enables the detection of energy‐resolved γ ‐ray spectra using a MAPbBr 3 single‐crystal device. Interestingly, the addition of formamidinium (FA) cations, which converted to methylformamidinium (MFA) cations by reaction with MA + during crystal growth further reduced MA defects. This enabled an energy resolution of 3.9% for the 662 keV 137 Cs line using a low bias of 100 V. The work provides direction toward enabling further improvements in wide‐bandgap perovskite‐based device performance by reducing detrimental defects.

Sponsoring Organization:
USDOE
OSTI ID:
2530485
Journal Information:
Advanced Materials, Journal Name: Advanced Materials Journal Issue: 35 Vol. 36; ISSN 0935-9648
Publisher:
Wiley Blackwell (John Wiley & Sons)Copyright Statement
Country of Publication:
Germany
Language:
English

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