Photoinduced singlet charge transfer in a ruthenium(II) perylene-3,4:9,10-bis(dicarboximide) complex

Victoria L. Gunderson, Elisha Krieg, Michael T. Vagnini, Mark A. Iron, Boris Rybtchinski, Michael R. Wasielewski

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31 Citations (Scopus)

Abstract

Elucidation of photoinduced charge transfer behavior in organic dye/metal hybrids is important for developing photocatalytic systems for solar energy conversion. We report the synthesis and photophysical characterization of a perylene-3,4:9,10-bis(dicarboximide) (PDI)-ruthenium(II) complex, bis-PDI-2,2′-bipyridineRu(II)Cl2(CNtbutyl) 2, which has favorable energetics, ΔGCS ≈ -1.0 eV, for singlet electron transfer from the Ru complex to PDI. Time-resolved optical spectroscopy reveals that upon selective photoexcitation of PDI, ultrafast charge transfer (<150 fs) from the Ru complex to 1*PDI generates the Ru(III)-PDI-• ion pair. The resulting vibrationally hot Ru(III)-PDI-• ion pair exhibits fast relaxation (τ = 3.9 ps) and charge recombination (τCR = 63 ps). Our experimental and computational (DFT and TDDFT) studies show that energy-preserving photodriven singlet electron transfer can dominate in properly designed organic dye/metal complexes, making them of particular interest for use in artificial photosynthetic systems for solar fuels formation.

Original languageEnglish
Pages (from-to)7533-7540
Number of pages8
JournalJournal of Physical Chemistry B
Volume115
Issue number23
DOIs
Publication statusPublished - Jun 16 2011

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ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films
  • Materials Chemistry

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