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

Motonobu Murakami, Kei Ohkubo, Taku Hasobe, Vito Sgobba, Dirk M. Guldi, Florian Wessendorf, Andreas Hirsch, Shunichi Fukuzumi

研究成果: Article査読

18 被引用数 (Scopus)

抄録

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.

本文言語English
ページ(範囲)1457-1466
ページ数10
ジャーナルJournal of Materials Chemistry
20
8
DOI
出版ステータスPublished - 2010

ASJC Scopus subject areas

  • 化学 (全般)
  • 材料化学

フィンガープリント

「Implementation of redox gradients in hydrogen bonded complexes containing N,N-dimethylaniline, flavin and fullerene derivatives」の研究トピックを掘り下げます。これらがまとまってユニークなフィンガープリントを構成します。

引用スタイル