0000000000048532

AUTHOR

And Arkady P. Yartsev

Interligand Electron Transfer Determines Triplet Excited State Electron Injection in RuN3−Sensitized TiO2 Films

Electron injection from the transition metal complex Ru(dcbpy)(2)(NCS)(2) (dcbpy = 2,2'-bipyridine-4,4'-dicarboxylate) into a titanium dioxide nanoparticle film occurs along two pathways. The dominating part of the electron injection proceeds from the initially excited singlet state of the sensitizer into the conduction band of the semiconductor on the sub-hundred-femtosecond time scale. The slower part of the injection occurs from the thermalized triplet excited state on the picosecond time scale in a nonexponential fashion, as was shown in a previous study (Benko, G.; et al. J. Am. Chem. Soc. 2002, 124, 489). Here we show that the slower channel of injection is the result of the excited s…

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Photoinduced ultrafast dye-to-semiconductor electron injection from nonthermalized and thermalized donor states.

Electron injection from the transition metal complex Ru(dcbpy)(2)(NCS)(2) (dcbpy = 4,4'-dicarboxy-2,2'-bipyridine) into a titanium dioxide nanocrystalline film occurs on the femto- and picosecond time scales. Here we show that the dominating part of the electron transfer proceeds extremely rapidly from the initially populated, vibronically nonthermalized, singlet excited state, prior to electronic and nuclear relaxation of the molecule. The results are especially relevant to the understanding and design of molecular-based photovoltaic devices and artificial photosynthetic assemblies.

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