Probing conformational dynamics in single donor-acceptor synthetic molecules by means of photoinduced reversible electron transfer

Proceedings of the National Academy of Sciences of the United States of America
Mircea CotletFrans C De Schryver

Abstract

We use single-molecule fluorescence lifetimes to probe dynamics of photoinduced reversible electron transfer occurring between triphenylamine (donor) and perylenediimide (acceptor) in single molecules of a polyphenylenic rigid dendrimer embedded in polystyrene. Here, reversible electron transfer in individual donor-acceptor molecules results in delayed fluorescence that is emitted with a high photon count rate. By monitoring fluorescence decay times on a photon-by-photon basis, we find fluctuations in both forward and reverse electron transfer spanning a broad time range, from milliseconds to seconds. Fluctuations are induced by conformational changes in the dendrimer structure as well by polystyrene chain reorientation. The conformational changes are related to changes in the dihedral angle of adjacent phenyl rings located in the dendritic branch near the donor transferring the charge, a torsional motion that results in millisecond fluctuations in the "through-bond" donor-acceptor electronic coupling. Polymer chain reorientation leads to changes in the local polarity experienced by the donors and to changes in the solvation of the charge-separated state. As a result, switching between different donor moieties within the same s...Continue Reading

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Citations

Jun 21, 2011·Journal of the American Chemical Society·Thi-Thanh-Tam NguyenKlaus Müllen
Jan 10, 2012·Journal of the American Chemical Society·Mirella El GemayelPaolo Samorì
Apr 4, 2007·Photochemical & Photobiological Sciences : Official Journal of the European Photochemistry Association and the European Society for Photobiology·Toby D M BellFrans C De Schryver
May 10, 2008·Photochemical & Photobiological Sciences : Official Journal of the European Photochemistry Association and the European Society for Photobiology·Eduard FronFrans C De Schryver
Apr 2, 2009·Photochemical & Photobiological Sciences : Official Journal of the European Photochemistry Association and the European Society for Photobiology·Jan VogelsangPhilip Tinnefeld
May 13, 2009·Proceedings of the National Academy of Sciences of the United States of America·Jan VogelsangPhilip Tinnefeld
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