Demonstration of energy-resolved γ-ray detection at room temperature by the CsPBCl3 perovskite semiconductor

Yihui He, Constantinos C. Stoumpos, Ido Hadar, Zhongzhen Luo, Kyle M. McCall, Zhifu Liu, Duck Young Chung, Bruce W. Wessels, Mercouri G. Kanatzidis*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

Abstract

The detection of γ-rays at room temperature with high-energy resolution using semiconductors is one of the most challenging applications. The presence of even the smallest amount of defects is sufficient to kill the signal generated from γ-rays which makes the availability of semiconductors detectors a rarity. Lead halide perovskite semiconductors exhibit unusually high defect tolerance leading to outstanding and unique optoelectronic properties and are poised to strongly impact applications in photoelectric conversion/detection. Here we demonstrate for the first time that large size single crystals of the all-inorganic perovskite CsPbCl3 semiconductor can function as a high-performance detector for γ-ray nuclear radiation at room temperature. CsPbCl3 is a wide-gap semiconductor with a bandgap of 3.03 eV and possesses a high effective atomic number of 69.8. We identified the two distinct phase transitions in CsPbCl3, from cubic (Pm-3m) to tetragonal (P4/mbm) at 325 K and finally to orthorhombic (Pbnm) at 316 K. Despite crystal twinning induced by phase transitions, CsPbCl3 crystals in detector grade can be obtained with high electrical resistivity of ∼1.7 × 109 Ω·cm. The crystals were grown from the melt with volume over several cubic centimeters and have a low thermal conductivity of 0.6 W m-1 K-1. The mobilities for electron and hole carriers were determined to ∼30 cm2/(V s). Using photoemission yield spectroscopy in air (PYSA), we determined the valence band maximum at 5.66 ± 0.05 eV. Under γ-ray exposure, our Schottky-type planar CsPbCl3 detector achieved an excellent energy resolution (∼16% at 122 keV) accompanied by a high figure-of-merit hole mobility-lifetime product (3.2 × 10-4 cm2/V) and a long hole lifetime (16 μs). The results demonstrate considerable defect tolerance of CsPbCl3 and suggest its strong potential for γ-radiation and X-ray detection at room temperature and above.

Original languageEnglish (US)
Pages (from-to)2068-2077
Number of pages10
JournalJournal of the American Chemical Society
Volume143
Issue number4
DOIs
StatePublished - Feb 3 2021

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

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