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Cu–F Interactions between Cationic Linear N-Heterocyclic Carbene Copper(I) Pyridine Complexes and Their Counterions Greatly Enhance Blue Luminescence Efficiency
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    Cu–F Interactions between Cationic Linear N-Heterocyclic Carbene Copper(I) Pyridine Complexes and Their Counterions Greatly Enhance Blue Luminescence Efficiency
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    • Annika Liske
      Annika Liske
      Institut für Anorganische Chemie, Universität Düsseldorf, Universitätsstrasse 1, 40225 Düsseldorf, Germany
      More by Annika Liske
    • Lars Wallbaum
      Lars Wallbaum
      Institut für Anorganische Chemie, Universität Düsseldorf, Universitätsstrasse 1, 40225 Düsseldorf, Germany
    • Torsten Hölzel
      Torsten Hölzel
      Institut für Anorganische Chemie, Universität Düsseldorf, Universitätsstrasse 1, 40225 Düsseldorf, Germany
    • Jelena Föller
      Jelena Föller
      Institut für Theoretische Chemie und Computerchemie, Universität Düsseldorf, Universitätsstrasse 1, 40225 Düsseldorf, Germany
    • Markus Gernert
      Markus Gernert
      Faculty for Chemistry and Chemical Biology, TU Dortmund University, Otto-Hahn-Strasse 6, 44227 Dortmund, Germany
    • Benjamin Hupp
      Benjamin Hupp
      Faculty for Chemistry and Chemical Biology, TU Dortmund University, Otto-Hahn-Strasse 6, 44227 Dortmund, Germany
    • Christian Ganter*
      Christian Ganter
      Institut für Anorganische Chemie, Universität Düsseldorf, Universitätsstrasse 1, 40225 Düsseldorf, Germany
      *E-mail: [email protected]
    • Christel M. Marian*
      Christel M. Marian
      Institut für Theoretische Chemie und Computerchemie, Universität Düsseldorf, Universitätsstrasse 1, 40225 Düsseldorf, Germany
      *E-mail: [email protected]
    • Andreas Steffen*
      Andreas Steffen
      Faculty for Chemistry and Chemical Biology, TU Dortmund University, Otto-Hahn-Strasse 6, 44227 Dortmund, Germany
      *E-mail: [email protected]
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    Inorganic Chemistry

    Cite this: Inorg. Chem. 2019, 58, 9, 5433–5445
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    https://doi.org/10.1021/acs.inorgchem.9b00337
    Published April 19, 2019
    Copyright © 2019 American Chemical Society

    Abstract

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    A series of easily accessible linear N-heterocyclic carbene (NHC) copper(I) complexes, bearing pyridine (py) and its derivatives as chromophore ligands, are barely emissive in the single-crystalline solid state. However, their powders, neat films, and dilute doped films of poly(methyl methacrylate) (PMMA; 1–10%) show very intense blue-to-blue-green photoluminescence with remarkable quantum yields φ of up to 87% and microsecond lifetimes, indicative of triplet states being involved. These luminescence properties are similar to trigonal coordinated NHC copper(I) bis(pyridine) complexes, which we have also isolated and characterized with respect to their structures and photophysics. Our spectroscopic and theoretical studies provide detailed insight into the nature of the luminescence enhancing effect of the linear two-coordinated copper(I) compounds, which is based on the formation of Cu–F interactions between the BF4 anions and [Cu(NHC)(2-R-py)]+ (R = H, Me, Ph) cations. These interactions are absent in the single crystals but lead to a distorted ground-state structure in the precipitated powders or in PMMA films, giving rise to high kr. In addition, we found that our linear copper(I) complexes exhibit mechanochromic luminescence because grinding of the single crystals leads to enhanced emission intensity. In light of the recently reported cation–anion contact-induced mechanochromic luminescence of two-coordinated copper(I) complexes, this study supports the generality of this new mechanism for the design of mechanoresponsive phosphorescent materials.

    Copyright © 2019 American Chemical Society

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.inorgchem.9b00337.

    • Further photophysical measurements, coordinates used for DFT/MRCI studies, and NMR and HRMS spectra (PDF)

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    CCDC 15106881510690 and 18768441876846 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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    Inorganic Chemistry

    Cite this: Inorg. Chem. 2019, 58, 9, 5433–5445
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.inorgchem.9b00337
    Published April 19, 2019
    Copyright © 2019 American Chemical Society

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