Proceedings of September Meeting 2016 (NFM16)
Publication date: 14th June 2016
Inspired by natural antenna complexes, DNA-hosted multi-chromophore systems (MCS’s) appear as a novel and convincing approach to assemble and study light-harvesting antennas for supramolecular devices with very high absorption cross-section and able to achieve efficient energy and charge transfer over several nm. In this study we investigate a family of DNA-MCS’s designed for light harvesting based on π-stacked Phenanthrenes in a DNA scaffold. A strong and robust coupling gives rise to an energy transfer (EnT) with unitary quantum yield over several nm. Excited state dynamics of these systems are investigated by UV-Vis femtosecond (fs) transient absorption to clarify their photophysics, the relevant times and dynamics of EnT as well as the role of molecular environment on the EnT mechanism. We found that EnT takes place within our time resolution (i.e. <40 fs), accounting for the unitary quantum yield. We observed the formation upon excitation of transient delocalized states that last from a few 10s to 100s of fs depending on the presence of an energy acceptor, suggesting that these states could mediate the EnT. To our knowledge, such a mechanism has never been proposed before, and contradicts the common opinion that efficient energy and charge transfers need long-lived states.
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