α-Particle Detection and Charge Transport Characteristics in the A3M2I9 Defect Perovskites (A = Cs, Rb; M = Bi, Sb)

McCall, Kyle M.; Liu, Zhifu; Trimarchi, Giancarlo; Stoumpos, Constantinos C.; Lin, Wenwen; He, Yihui; Hadar, Ido; Kanatzidis, Mercouri G.; Wessels, Bruce W.

doi:10.1021/acsphotonics.8b00813

Title: α-Particle Detection and Charge Transport Characteristics in the A₃M₂I₉ Defect Perovskites (A = Cs, Rb; M = Bi, Sb)

Journal Article · Wed Aug 08 00:00:00 EDT 2018 · ACS Photonics

DOI:https://doi.org/10.1021/acsphotonics.8b00813· OSTI ID:1494818

^[1]; Liu, Zhifu ^[2]; Trimarchi, Giancarlo ^[3];

^[3];

^[2]

Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry, and Dept. of Materials Science and Engineering
Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering
Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry

Here, we have investigated the defect perovskites A₃M₂I₉ (A = Cs, Rb; M = Bi, Sb) as materials for radiation detection. The phase purity of Bridgman-grown A₃M₂I₉ single crystals was confirmed via high-resolution synchrotron X-ray diffraction, while density functional theory calculations (DFT) show surprisingly dispersive bands in the out-of-plane direction for these layered materials, with low effective masses for both holes and electrons. Accordingly, each of the four A₃M₂I₉ defect perovskites showed response to ²⁴¹Am α-particle irradiation for hole and electron electrode configurations, a remarkable ambipolar response that resembles the 3D halide perovskites. The electron response spectra were used to estimate the mobility–lifetime product (μτ)_e for electrons in these materials, with Rb₃Bi₂I₉ showing the lowest (μτ)_e value of 1.7 × 10^–6 cm² V^–1 and Cs₃Bi₂I₉ the highest (μτ)_e of 5.4 × 10^–5 cm² V^–1. The rise time of the α-particle-generated pulse was used to estimate the electron mobility μ_e of the A₃M₂I₉ defect perovskites, which ranged from 0.32 cm² V^–1s–1 for Rb₃Sb₂I₉ to 4.3 cm² V^–1s^–1 in Cs₃Bi₂I₉. Similar analysis of the hole response spectra yielded (μτ)_h values for each A₃M₂I₉ compound, with Cs₃Bi₂I₉ again showing the highest (μτ)_h value of 1.8 × 10^–5 cm² V^–1, while Rb₃Bi₂I₉ showed the lowest (μτ)_h with 2.0 × 10^–6 cm₂ V^–1. Rise time analysis gave hole mobilities ranging from 1.7 cm² V^–1 s^–1 for Cs₃Bi₂I₉ to 0.14 cm² V^–1 s^–1 for Cs₃Sb₂I₉. Comparing the experimental electron and hole mobilities to the effective masses obtained from DFT calculations revealed sizable discrepancies, possibly indicating self-trapping of charge carriers due to electron–phonon interactions. The α-particle response of the A₃M₂I₉ defect perovskites demonstrates their potential as semiconductor radiation detectors, with Cs₃Bi₂I₉ and Cs₃Sb₂I₉ showing the most promise.

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Research Organization:: Northwestern Univ., Evanston, IL (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: NA0002522

OSTI ID:: 1494818

Journal Information:: ACS Photonics, Vol. 5, Issue 9; ISSN 2330-4022

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 67 works

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
charge transport
halide perovskite
radiation detection
semiconductor detector

Title: α-Particle Detection and Charge Transport Characteristics in the A3M2I9 Defect Perovskites (A = Cs, Rb; M = Bi, Sb)

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Title: α-Particle Detection and Charge Transport Characteristics in the A₃M₂I₉ Defect Perovskites (A = Cs, Rb; M = Bi, Sb)