Soft Lattice and Defect Covalency Rationalize Tolerance of β‐CsPbI 3 Perovskite Solar Cells to Native Defects

Chu, Weibin; Saidi, Wissam A.; Zhao, Jin; Prezhdo, Oleg V.

doi:10.1002/anie.201915702

Soft Lattice and Defect Covalency Rationalize Tolerance of β‐CsPbI ₃ Perovskite Solar Cells to Native Defects

Journal Article · Tue Feb 18 23:00:00 EST 2020 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.201915702· OSTI ID:1600839

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Departments of Chemistry, and Physics and Astronomy University of Southern California Los Angeles CA 90089 USA
Department of Mechanical Engineering and Materials Science University of Pittsburgh Pittsburgh PA 15261 USA
ICQD/Hefei National Laboratory for Physical Sciences at the Microscale CAS Key Laboratory of Strongly-Coupled Quantum Matter Physics, and Department of Physics University of Science and Technology of China Hefei Anhui 230026 China, Department of Physics and Astronomy University of Pittsburgh Pittsburgh PA 15260 USA, Synergetic Innovation Center of Quantum Information &, Quantum Physics University of Science and Technology of China Hefei Anhui 230026 China

Abstract

Although all‐inorganic metal halide perovskites (MHPs) have shown tremendous improvement, they are still inferior to the hybrid organic–inorganic MHPs in efficiency. Recently, a conceptually new β‐CsPbI ₃ perovskite reached 18.4 % efficiency combined with good thermodynamic stability at ambient conditions. We use ab initio non‐adiabatic molecular dynamics to show that native point defects in β‐CsPbI ₃ are generally benign for nonradiative charge recombination, regardless of whether they introduce shallow or deep trap states. These results indicate that MHPs do not follow the simple models used to explain defect‐mediated charge recombination in the conventional semiconductors. The strong tolerance is due to the softness of the perovskite lattice, which permits separation of electrons and holes upon defect formation, and only allows carriers to couple to the low‐frequency vibrations. Both factors decrease notably the non‐adiabatic coupling and slow down the dissipation of energy to heat.

View Accepted Manuscript (Publisher)

Sponsoring Organization:: USDOE

Grant/Contract Number:: SC0014429

OSTI ID:: 1600839

Alternate ID(s):: OSTI ID: 1802646
OSTI ID: 22947266

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 16 Vol. 59; ISSN 1433-7851

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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