Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 10, Issue 3, Pages 595-602Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.200305408
Keywords
dyes/pigments; electron transfer; ruthenium; supramolecular chemistry
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A [Ru(dcbpy)(2)(NCS)(2)] dye has been chemically modified by the addition of a secondary electron donor moiety, N,N-(di-p-anisylamino)phenoxymethyl. Optical excitation of the modified dye adsorbed to nanocrystalline TiO2 films shows a remarkably long-lived charge-separated state, with a decay half time of 0.7 s. Semiempirical calculations confirm that the HOMO of the modified dye molecule is localised on the electron donor group. The retardation of the recombination dynamics relative to the unmodified control dye is caused by the increase in the spatial separation of the HOMO orbital from the TiO2 surface. The magnitude of the retardation is shown to be in agreement with that predicted from the non-adiabatic electron-tunnelling theory.
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