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    Polar Nature of (CH3NH3)3Bi2I9 Perovskite-Like Hybrids
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    † Zernike Institute for Advanced Materials, University of Groningen, Nijenborgh 4, Groningen 9747 AG, The Netherlands
    ‡ Consiglio Nazionale della Ricerche (CNR-SPIN), Via Vetoio 10, L’Aquila 67100, Italy
    § Research Centre for Thermogravimetric and Calorimetric Research, St. Petersburg State University, 7/9 Universitetskaya nab., St. Petersburg 199034, Russia
    ∥ Institute of Chemistry, St. Petersburg State University, Universitetskiy prospect 26, Petrodvoretz, St. Petersburg 198504, Russia
    *E-mail: [email protected]
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    Inorganic Chemistry

    Cite this: Inorg. Chem. 2017, 56, 1, 33–41
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    https://doi.org/10.1021/acs.inorgchem.6b01699
    Published September 14, 2016
    Copyright © 2016 American Chemical Society
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    High-quality single crystals of perovskite-like (CH3NH3)3Bi2I9 hybrids have been synthesized, using a layered-solution crystal-growth technique. The large dielectric constant is strongly affected by the polar ordering of its constituents. Progressive dipolar ordering of the methylammonium cation upon cooling below 300 K gradually converts the hexagonal structure (space group P63/mmc) into a monoclinic phase (C2/c) at 160 K. A well-pronounced, ferrielectric phase transition at 143 K is governed by in-plane ordering of the bismuth lone pair that breaks inversion symmetry and results in a polar phase (space group P21). The dielectric constant is markedly higher in the C2/c phase above this transition. Here, the bismuth lone pair is disordered in-plane, allowing the polarizability to be substantially enhanced. Density functional theory calculations estimate a large ferroelectric polarization of 7.94 μC/cm2 along the polar axis in the P21 phase. The calculated polarization has almost equal contributions of the methylammonium and Bi3+ lone pair, which are fairly decoupled.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.inorgchem.6b01699.

    • DSC data, thermal ellipsoid figures, reciprocal lattice planes, and absorption data (PDF)

    • Crystallographic information files of (CH3NH3)3Bi2I9 at 100, 160, and 300 K (CIF)

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    Inorganic Chemistry

    Cite this: Inorg. Chem. 2017, 56, 1, 33–41
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    https://doi.org/10.1021/acs.inorgchem.6b01699
    Published September 14, 2016
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