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A Vanadium(III) Complex with Blue and NIR-II Spin-Flip Luminescence in Solution

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    A Vanadium(III) Complex with Blue and NIR-II Spin-Flip Luminescence in Solution
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    • Matthias Dorn
      Matthias Dorn
      Department of Chemistry, Johannes Gutenberg University of Mainz, Duesbergweg 10-14, Mainz 55128, Germany
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    • Jens Kalmbach
      Jens Kalmbach
      Institute of Inorganic Chemistry, University of Tübingen, Auf der Morgenstelle 18, Tübingen 72076, Germany
      More by Jens Kalmbach
    • Pit Boden
      Pit Boden
      Department of Chemistry and Research Center Optimas, TU Kaiserslautern, Erwin-Schrödinger-Straße, Kaiserslautern 67663, Germany
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    • Ayla Päpcke
      Ayla Päpcke
      Institute for Physics and Department of Life, Light and Matter, University of Rostock, Rostock 18051, Germany
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    • Sandra Gómez
      Sandra Gómez
      Institute of Theoretical Chemistry, Faculty of Chemistry, University of Vienna, Währinger Straße 17, Vienna 1090, Austria
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    • Christoph Förster
      Christoph Förster
      Department of Chemistry, Johannes Gutenberg University of Mainz, Duesbergweg 10-14, Mainz 55128, Germany
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    • Felix Kuczelinis
      Felix Kuczelinis
      Department of Chemistry, Johannes Gutenberg University of Mainz, Duesbergweg 10-14, Mainz 55128, Germany
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    • Luca M. Carrella
      Luca M. Carrella
      Department of Chemistry, Johannes Gutenberg University of Mainz, Duesbergweg 10-14, Mainz 55128, Germany
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    • Laura A. Büldt
      Laura A. Büldt
      Institute of Inorganic Chemistry, University of Tübingen, Auf der Morgenstelle 18, Tübingen 72076, Germany
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    • Nicolas H. Bings
      Nicolas H. Bings
      Department of Chemistry, Johannes Gutenberg University of Mainz, Duesbergweg 10-14, Mainz 55128, Germany
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    • Eva Rentschler
      Eva Rentschler
      Department of Chemistry, Johannes Gutenberg University of Mainz, Duesbergweg 10-14, Mainz 55128, Germany
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      Orcidhttp://orcid.org/0000-0003-1431-3641
    • Stefan Lochbrunner
      Stefan Lochbrunner
      Institute for Physics and Department of Life, Light and Matter, University of Rostock, Rostock 18051, Germany
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    • Leticia González
      Leticia González
      Institute of Theoretical Chemistry, Faculty of Chemistry, University of Vienna, Währinger Straße 17, Vienna 1090, Austria
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      Orcidhttp://orcid.org/0000-0001-5112-794X
    • Markus Gerhards*
      Markus Gerhards
      Department of Chemistry and Research Center Optimas, TU Kaiserslautern, Erwin-Schrödinger-Straße, Kaiserslautern 67663, Germany
      *[email protected]
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      Orcidhttp://orcid.org/0000-0002-8748-2940
    • Michael Seitz*
      Michael Seitz
      Institute of Inorganic Chemistry, University of Tübingen, Auf der Morgenstelle 18, Tübingen 72076, Germany
      *[email protected]
      More by Michael Seitz
      Orcidhttp://orcid.org/0000-0002-9313-2779
    • Katja Heinze*
      Katja Heinze
      Department of Chemistry, Johannes Gutenberg University of Mainz, Duesbergweg 10-14, Mainz 55128, Germany
      *[email protected]
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      Orcidhttp://orcid.org/0000-0003-1483-4156
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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2020, 142, 17, 7947–7955
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    https://doi.org/10.1021/jacs.0c02122
    Published April 10, 2020
    Copyright © 2020 American Chemical Society
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    Abstract

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    Luminescence from Earth-abundant metal ions in solution at room temperature is a very challenging objective due to the intrinsically weak ligand field splitting of first-row transition metal ions, which leads to efficient nonradiative deactivation via metal-centered states. Only a handful of 3dn metal complexes (n ≠ 10) show sizable luminescence at room temperature. Luminescence in the near-infrared spectral region is even more difficult to achieve as further nonradiative pathways come into play. No Earth-abundant first-row transition metal complexes have displayed emission >1000 nm at room temperature in solution up to now. Here, we report the vanadium(III) complex mer-[V(ddpd)2][PF6]3 yielding phosphorescence around 1100 nm in valeronitrile glass at 77 K as well as at room temperature in acetonitrile with 1.8 × 10–4% quantum yield (ddpd = N,N′-dimethyl-N,N′-dipyridine-2-ylpyridine-2,6-diamine). In addition, mer-[V(ddpd)2][PF6]3 shows very strong blue fluorescence with 2% quantum yield in acetonitrile at room temperature. Our comprehensive study demonstrates that vanadium(III) complexes with d2 electron configuration constitute a new class of blue and NIR-II luminophores, which complement the classical established complexes of expensive precious metals and rare-earth elements.

    Copyright © 2020 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/jacs.0c02122.

    • Data of quantum chemical calculations, synthetic procedures, and analytical and spectroscopic data of [V(ddpd)2][PF6]3 (PDF)

    • X-ray crystallographic data for mer-[V(ddpd)2][PF6]3×3CH3CN (CIF)

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    Cite this: J. Am. Chem. Soc. 2020, 142, 17, 7947–7955
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