Angewandte Chemie - International Edition
Angewandte Chemie - International Edition
5 years ago

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

Time-Resolved Interception of Multiple-Charge Accumulation in a Sensitizer–Acceptor Dyad
Thomas Pino, Van-Thai Pham, Thierry Chamaillé, Christophe Lefumeux, Annamaria Quaranta, Minh-Huong Ha-Thi, Stéphanie Mendes Marinho, Winfried Leibl, Ally Aukauloo
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). A molecular dyad containing a naphthalene diimide (NDI) linked to a [Ru(bpy)3]2+ (bpy=bipyridine) chromophore by a reversible electron donor is used in a double-excitation nanosecond pump–pump–probe experiment to investigate two successive rounds of photoinduced electron transfer. An unprecedented long-lived two-electron charge accumulation occurs. css=charge-separated state.

Publisher URL: http://onlinelibrary.wiley.com/resolve/doi

DOI: 10.1002/anie.201706564

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