Engaging Copper(III) Corrole as an Electron Acceptor: Photoinduced Charge Separation in Zinc Porphyrin–Copper Corrole Donor–Acceptor Conjugates

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  • Thien H. Ngo
    International Center for Young Scientist (ICYS) National Institute for Materials Science Namiki 1-1 Tsukuba Ibaraki 305-0044 Japan
  • David Zieba
    Institut für Chemie und Biochemie Freie Universität Berlin Takustrasse 3 14195 Berlin Germany
  • Whitney A. Webre
    Department of Chemistry University of North Texas 1155 Union Circle, 305070 Denton TX 76203 USA
  • Gary N. Lim
    Department of Chemistry University of North Texas 1155 Union Circle, 305070 Denton TX 76203 USA
  • Paul A. Karr
    Department of Physical Sciences and Mathematics Wayne State College 111 Main Street Wayne NE 68787 USA
  • Scheghajegh Kord
    Institut für Chemie und Biochemie Freie Universität Berlin Takustrasse 3 14195 Berlin Germany
  • Shangbin Jin
    WPI Center for Materials Nanoarchitectonics National Institute for Materials Science Namiki 1-1 Tsukuba Ibaraki 305-0044 (Japan
  • Katsuhiko Ariga
    WPI Center for Materials Nanoarchitectonics National Institute for Materials Science Namiki 1-1 Tsukuba Ibaraki 305-0044 (Japan
  • Marzia Galli
    Department of Chemistry University of Southampton Southampton SO17 1BJ UK
  • Steve Goldup
    Department of Chemistry University of Southampton Southampton SO17 1BJ UK
  • Jonathan P. Hill
    WPI Center for Materials Nanoarchitectonics National Institute for Materials Science Namiki 1-1 Tsukuba Ibaraki 305-0044 (Japan
  • Francis D'Souza
    Department of Chemistry University of North Texas 1155 Union Circle, 305070 Denton TX 76203 USA

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<jats:title>Abstract</jats:title><jats:p>An electron‐deficient copper(III) corrole was utilized for the construction of donor–acceptor conjugates with zinc(II) porphyrin (ZnP) as a singlet excited state electron donor, and the occurrence of photoinduced charge separation was demonstrated by using transient pump–probe spectroscopic techniques. In these conjugates, the number of copper corrole units was varied from 1 to 2 or 4 units while maintaining a single ZnP entity to observe the effect of corrole multiplicity in facilitating the charge‐separation process. The conjugates and control compounds were electrochemically and spectroelectrochemically characterized. Computational studies revealed ground state geometries of the compounds and the electron‐deficient nature of the copper(III) corrole. An energy level diagram was established to predict the photochemical events by using optical, emission, electrochemical, and computational data. The occurrence of charge separation from singlet excited zinc porphyrin and charge recombination to yield directly the ground state species were evident from the diagram. Femtosecond transient absorption spectroscopy studies provided spectral evidence of charge separation in the form of the zinc porphyrin radical cation and copper(II) corrole species as products. Rates of charge separation in the conjugates were found to be of the order of 10<jats:sup>10</jats:sup> s<jats:sup>−1</jats:sup> and increased with increasing multiplicity of copper(III) corrole entities. The present study demonstrates the importance of copper(III) corrole as an electron acceptor in building model photosynthetic systems.</jats:p>

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