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Time‐Resolved Interception of Multiple‐Charge Accumulation in a Sensitizer–Acceptor Dyad
Author(s) -
Mendes Marinho Stéphanie,
HaThi MinhHuong,
Pham VanThai,
Quaranta Annamaria,
Pino Thomas,
Lefumeux Christophe,
Chamaillé Thierry,
Leibl Winfried,
Aukauloo Ally
Publication year - 2017
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201706564
Subject(s) - chromophore , photochemistry , chemistry , charge (physics) , electron transfer , chemical physics , redox , nanosecond , photoinduced charge separation , bipyridine , electron acceptor , artificial photosynthesis , catalysis , physics , photocatalysis , crystallography , organic chemistry , quantum mechanics , laser , crystal structure , optics
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).