Assessment of dynamic structural instabilities across 24 cubic inorganic halide perovskites

Yang, Ruo Xi; Skelton, Jonathan M.; da Silva, Estelina L.; Frost, Jarvist M.; Walsh, Aron

doi:10.1063/1.5131575

Title: Assessment of dynamic structural instabilities across 24 cubic inorganic halide perovskites

Journal Article · 13 January 2020 · Journal of Chemical Physics

DOI: https://doi.org/10.1063/1.5131575 · OSTI ID:1603581

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Imperial College London, London (United Kingdom). Dept. of Materials; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry
Univ. of Manchester (United Kingdom). Dept. of Chemistry
Polytechnic Univ. of Valencia (UPV) (Spain). Inst. de Diseño para la Fabricación y Producción Automatizada
Imperial College London, London (United Kingdom). Dept. of Physics
Imperial College London, London (United Kingdom); Yonsei Univ., Seoul (South Korea)

Metal halide perovskites are promising candidates for next-generation photovoltaic and optoelectronic applications. The flexible nature of the octahedral network introduces complexity when understanding their physical behavior. It has been shown that these materials are prone to decomposition and phase competition, and the local crystal structure often deviates from the average space group symmetry. To make stable phase-pure perovskites, understanding their structure-composition relations is of central importance. We demonstrate, from lattice dynamics calculations, that the 24 inorganic perovskites ABX₃ (A = Cs, Rb; B = Ge, Sn, Pb; X = F, Cl, Br, I) exhibit instabilities in their cubic phase. These instabilities include cation displacements, octahedral tilting, and Jahn-Teller distortions. The magnitudes of the instabilities vary depending on the chemical identity and ionic radii of the composition. The tilting instabilities are energetically dominant and reduce as the tolerance factor increases, whereas cation displacements and Jahn-Teller type distortions depend on the interactions between the constituent ions. We further considered representative tetragonal, orthorhombic, and monoclinic perovskite phases to obtain phonon-stable structures for each composition. This work provides insights into the thermodynamic driving force of the instabilities and will help guide computer simulations and experimental synthesis in material screening.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC); EPSRC; National Research Foundation of Korea (NRF); European Union (EU)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1603581

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 2 Vol. 152; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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