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Implementation of redox gradients in hydrogen bonded complexes containing N,N-dimethylaniline, flavin and fullerene derivatives

Title
Implementation of redox gradients in hydrogen bonded complexes containing N,N-dimethylaniline, flavin and fullerene derivatives
Authors
Murakami M.Ohkubo K.Hasobe T.Sgobba V.Guldi D.M.Wessendorf F.Hirsch A.Fukuzumi S.
Ewha Authors
Shunichi Fukuzumi
SCOPUS Author ID
Shunichi Fukuzumiscopus
Issue Date
2010
Journal Title
Journal of Materials Chemistry
ISSN
0959-9428JCR Link
Citation
vol. 20, no. 8, pp. 1457 - 1466
Indexed
SCOPUS WOS scopus
Abstract
A variety of supramolecular complexes were formed by associating an electron donor-substituted flavin dyad (10-[4′-(N,N-dimethylamino)phenyl] isoalloxazine: DMA-Fl) and a family of fullerene derivatives that contain single and double hydrogen bond receptors (SRC60 and DRC60). The stoichiometry of the corresponding complexes, that is, DMA-Fl and SRC 60 or DRC60, were examined by Job's plot analysis of the absorption changes linked to DMA-Fl at 470 nm. To this end, 1:1 and 1:2 complex stoichiometries were determined for DMA-Fl-SRC60 and (DMA-Fl) 2-DRC60, respectively. Molecular aggregates in the form of remarkably stable clusters were formed by the fast injection method. Insights into these clusters came from transmission electron microscopy (TEM) measurements, which revealed network configurations for (DMA-Fl-SRC 60)n with diameters in the range between 200 and 500 nm, while uniform nanoparticles of about 40 nm diameter were discernible for [(DMA-Fl)2-DRC60]n. The highly colored composite clusters were assembled onto an optically transparent electrode covered with nanostructured SnO2 films by the electrophoretic deposition technique. Important are the photocurrent action spectra providing maximum IPCE values that are twice as high for [(DMA-Fl)2-DRC 60]n than for (DMA-Fl-SRC60)n. To complement these studies the dynamics of electron transfer were investigated by femtosecond laser flash photolysis in the supramolecular clusters (i.e., (DMA-Fl-SRC60)n and [(DMA-Fl)2-DRC 60]n). As a matter of fact, for the first time we were able to demonstrate the unidirectional electron transfer from the terminal electron donor (N,N-dimethylaniline) moiety to the terminal electron acceptor (fullerene) moiety. © The Royal Society of Chemistry 2010.
DOI
10.1039/b918462g
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자연과학대학 > 화학·나노과학전공 > Journal papers
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