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Two-Dimensional Lead(II) Halide-Based Hybrid Perovskites Templated by Acene Alkylamines: Crystal Structures, Optical Properties, and Piezoelectricity

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Download Hi-Res ImageDownload to MS-PowerPointCite This:Inorg. Chem. 2017, 56, 15, 9291-9302
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    Two-Dimensional Lead(II) Halide-Based Hybrid Perovskites Templated by Acene Alkylamines: Crystal Structures, Optical Properties, and Piezoelectricity
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    † ‡ †Department of Mechanical Engineering and Materials Science, ‡Department of Chemistry, and §Department of Biomedical Engineering, Duke University, Durham, North Carolina 27708, United States
    ∥ NSF Research Triangle Materials Research Science and Engineering Center, Durham, North Carolina 27708, United States
    *E-mail: [email protected]
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    Inorganic Chemistry

    Cite this: Inorg. Chem. 2017, 56, 15, 9291–9302
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    https://doi.org/10.1021/acs.inorgchem.7b01094
    Published July 27, 2017
    Copyright © 2017 American Chemical Society
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    Abstract

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    A series of two-dimensional (2D) hybrid organic–inorganic perovskite (HOIP) crystals, based on acene alkylamine cations (i.e., phenylmethylammonium (PMA), 2-phenylethylammonium (PEA), 1-(2-naphthyl)methanammonium (NMA), and 2-(2-naphthyl)ethanammonium (NEA)) and lead(II) halide (i.e., PbX42–, X = Cl, Br, and I) frameworks, and their corresponding thin films were fabricated and examined for structure–property relationship. Several new or redetermined crystal structures are reported, including those for (NEA)2PbI4, (NEA)2PbBr4, (NMA)2PbBr4, (PMA)2PbBr4, and (PEA)2PbI4. Non-centrosymmetric structures from among these 2D HOIPs were confirmed by piezoresponse force microscopy—especially noteworthy is the structure of (PMA)2PbBr4, which was previously reported as centrosymmetric. Examination of the impact of organic cation and inorganic layer choice on the exciton absorption/emission properties, among the set of compounds considered, reveals that perovskite layer distortion (i.e., Pb–I–Pb bond angle between adjacent PbI6 octahedra) has a more global effect on the exciton properties than octahedral distortion (i.e., variation of I–Pb–I bond angles and discrepancy among Pb–I bond lengths within each PbI6 octahedron). In addition to the characteristic sharp exciton emission for each perovskite, (PMA)2PbCl4, (PEA)2PbCl4, (NMA)2PbCl4, and (PMA)2PbBr4 exhibit separate, broad “white” emission in the long wavelength range. Piezoelectric compounds identified from these 2D HOIPs may be considered for future piezoresponse-type energy or electronic applications.

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    Supporting Information

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    The cif files for each of the new/redetermined structures, The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.inorgchem.7b01094.

    • Details of general molecule structure, crystal data and structure refinement parameters, the conformation and orientation of organic cations, raw data of optical absorption, more structure–property relationship figures and piezoresponse as a function of the driving frequency for the compounds not listed in the main text. The CCDC Nos. for (PMA)2PbBr4, (PEA)2PbI4, (NMA)2PbBr4, (NEA)2PbI4, and (NEA)2PbBr4 are 1542460, 1542461, 1542462, 1542463, and 1542464, respectively. (PDF)

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    CCDC 1542460–1542464 contain the supplementary crystallographic data for this paper. These data can be obtained free of charge via www.ccdc.cam.ac.uk/data_request/cif, or by emailing [email protected], or by contacting The Cambridge Crystallographic Data Centre, 12 Union Road, Cambridge CB2 1EZ, UK; fax: +44 1223 336033.

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    Cite this: Inorg. Chem. 2017, 56, 15, 9291–9302
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