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BEDT-TTF Salts Formed with Tetrahedrally Coordinated Zinc(II) Complex Anions

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    BEDT-TTF Salts Formed with Tetrahedrally Coordinated Zinc(II) Complex Anions
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    † Faculty of Agriculture, Meijo University, Tempaku-ku, Nagoya 468-8502, Japan
    ‡ Department of Applied Physics, Nagoya University, Chikusa-ku, Nagoya 464-8603, Japan
    § Division of Chemistry, Graduate School of Science, Kyoto University, Sakyo-ku, Kyoto 606-8502, Japan
    # Research Center for Low Temperature and Materials Sciences, Kyoto University, Sakyo-ku, Kyoto 606-8501, Japan
    ∥ Toyota Physical and Chemical Research Institute, Nagakute 480-1192, Japan
    *Phone: +81-52-838-2552. Fax: +81-52-833-7200. E-mail: [email protected]
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    Crystal Growth & Design

    Cite this: Cryst. Growth Des. 2016, 16, 11, 6613–6630
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    https://doi.org/10.1021/acs.cgd.6b01294
    Published September 27, 2016
    Copyright © 2016 American Chemical Society
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    Abstract

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    Twelve kinds of bis(ethylenedithio)tetrathiafulvalene (BEDT-TTF or ET) cation radical salts with tetrahedrally coordinated zinc(II) complex anions were obtained by electrocrystallization; most of them were produced via the additional reaction of Lewis-basic cyano-containing anions [N(CN)2–, C(CN)3–, and Au(CN)2–] with ZnX2 (X = Cl–, Br–, and SCN–) that occurred during electrocrystallization. On the basis of the charge and arrangement of ET molecules, these salts were predominantly categorized into four groups: (A) isolated ET•+ dimers or tetramers, (B) infinite ET•+ ribbon, (C) infinite layers either with a peculiar ET0.5+ arrangement of ET molecules with partial charges other than +0.5, and (D) infinite layers of ET0.5+ molecules. In A, zinc(II) complex anions including a unidentate-coordinated C(CN)3 or Au(CN)2 group spatially interrupt the infinite arrangement of ET molecules. The ET•+ ribbon in B runs parallel to the pseudopolymeric chain of disordered Zn[C(CN)3]2Br22– ions. In C, two salts are semiconductive, whereas the remaining two salts behave as metallic at room temperature and undergo a metal–insulator transition on cooling. The ET molecules in D are arranged in a θ42+40-like packing motif, due to the nonplanar anionic layers. All salts are semiconductive and exhibit a gradual evolution in their superstructures with cooling associated with charge disproportionation.

    Copyright © 2016 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.cgd.6b01294.

    • Calculated band structure for 6 (Figure S1), temperature dependence of the intensity at the superlattice Bragg positions for 10–12 (Figure S2) (PDF)

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    CCDC 1482867–1482883 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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    5. Ivan Potočňák, Oleksandr Bukrynov, Andrii Kliuikov, Erik Čižmár, Svitlana Vitushkina, Lucia Váhovská, Erika Samoľová. Low-dimensional compounds containing cyanido groups. Part XXXIV. Structure, spectral and magnetic properties of the first complex with pyridylbenzimidazole and nonlinear pseudohalide anion. Zeitschrift für Kristallographie - Crystalline Materials 2018, 233 (12) , 877-882. https://doi.org/10.1515/zkri-2018-2091
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    Crystal Growth & Design

    Cite this: Cryst. Growth Des. 2016, 16, 11, 6613–6630
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.cgd.6b01294
    Published September 27, 2016
    Copyright © 2016 American Chemical Society
    Request reuse permissions

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