Centimeter-Sized 2D Perovskitoid Single Crystals for Efficient X-ray Photoresponsivity

Chuang Ma, Lili Gao*, Zhuo Xu, Xiaotong Li, Xin Song, Yucheng Liu, Tinghuan Yang, Haojin Li, Yachao Du, Guangtao Zhao, Xinmei Liu, Mercouri G. Kanatzidis, Shengzhong Frank Liu, Kui Zhao

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

Abstract

Metal-halide perovskitoids with corner-, edge-, and face-sharing octahedra provide a fertile “playground” for structure modulation. With low defect density, low ion migration, and high intrinsic stability, two-dimensional (2D) perovskitoid single crystals are expected to be ideal materials for room-temperature semiconductor detectors (RTSDs) as high-energy radiation. However, there is no report yet on the use of 2D perovskitoid single crystals for X-ray detection, as well as on how the halide-modulated molecular assembly would affect their structure and properties. Herein, based on an amidino-based organic spacer, we successfully synthesized a novel family of centimeter-sized 2D perovskitoid single crystals, (3AP)PbX4 (3AP = 3-amidinopyridine, X = Cl, Br, and I). This is the first time that centimeter-sized 2D perovskitoid single crystals are demonstrated for X-ray photoresponse. Detailed investigations reveal a unique crystal packing with corner-sharing and edge-sharing octahedra of inorganic frameworks and 3AP cations lying between adjacent inorganic layers in a parallel and antisymmetric manner. Changing the halide from I to Br and Cl results in greater Pb-X-Pb angles and stronger hydrogen bonding in perovskitoids and therefore consequently a better elastic recovery under stress, a more efficient charge transport in the inorganic layer, and a lower ionic migration. By varying halide substitution, an efficient X-ray photoresponse is achieved with a sensitivity up to 791.8 μC Gyair-1 cm-2 for (3AP)PbCl4 and a low detection limit of 1.54 μGyair s-1. These results reveal that the large 2D perovskitoid single crystals provide a promising platform for high performance optoelectronics.

Original languageEnglish (US)
Pages (from-to)1699-1709
Number of pages11
JournalChemistry of Materials
Volume34
Issue number4
DOIs
StatePublished - Feb 22 2022

ASJC Scopus subject areas

  • Chemistry(all)
  • Chemical Engineering(all)
  • Materials Chemistry

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