Time-Resolved Interception of Multiple-Charge Accumulation in a Sensitizer–Acceptor Dyad

Stéphanie Mendes Marinho, Minh Huong Ha-Thi, Van Thai Pham, Annamaria Quaranta, Thomas Pino, Christophe Lefumeux, Thierry Chamaillé, Winfried Leibl, Ally Aukauloo

Research output: Contribution to journalArticlepeer-review

32 Citations (SciVal)

Abstract

Biomimetic models that contain elements of photosynthesis are fundamental in the development of synthetic systems that can use sunlight to produce fuel. The critical task consists of running several rounds of light-induced charge separation, which is required to accumulate enough redox equivalents at the catalytic sites for the target chemistry to occur. Long-lived first charge-separated state and distinct electronic signatures for the sequential charge accumulated species are essential features to be able to track these events on a spectroscopic ground. Herein, we use a double-excitation nanosecond pump–pump–probe experiment to interrogate two successive rounds of photo-induced electron transfer on a molecular dyad containing a naphthalene diimide (NDI) linked to a [Ru(bpy)3]2+ (bpy=bipyridine) chromophore by using a reversible electron donor. We report an unprecedented long-lived two-electron charge accumulation (t=200 μs).

Original languageEnglish
Pages (from-to)15936-15940
Number of pages5
JournalAngewandte Chemie - International Edition
Volume56
Issue number50
DOIs
Publication statusPublished - 2017 Dec 11

Subject classification (UKÄ)

  • Biochemistry and Molecular Biology

Keywords

  • electron transfer
  • energy conversion
  • molecular dyads
  • photosynthesis
  • time-resolved spectroscopy

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