Journal
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
Volume 185, Issue 2-3, Pages 331-337Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.jphotochem.2006.06.028
Keywords
high molar extinction coefficient charge transfer sensitizer; nanocrystalline TiO2 films; dye-sensitized solar cells; ruthenium sensitizer; heteroleptic ruthenium complex
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A high molar extinction coefficient charge transfer sensitizer tetrabutylammonium [Ru(4,-carboxylic acid-4'-carboxylate-2,2'-bipyridine)(4,4'di-(2-(3,6-dimethoxyphenyl)ethenyl)-2,2'-bipyridine)(NCS)(2)], is developed which upon anchoring onto nanocrystalline TiO2 films exhibit superior power conversion efficiency compared to the standard sensitizer bistetrabutylammonium cis-dithiocyanatobis(4,4'-dicarboxylic acid-2,2'bipyridine)ruthenium(II) (N719). The new sensitizer anchored TiO2 films harvest visible light very efficiently over a large spectral range and produce a short-circuit photocurrent density of 18.84 mA/cm(2), open-circuit voltage 783 mV and fill factor 0.73, resulting remarkable solar-to-electric energy conversion efficiency (eta) 10.82, under Air Mass (AM) 1.5 sunlight. The Time Dependent Density Functional Theory (TDDFT) excited state calculations of the new sensitizer show that the first three HOMOs have ruthenium t(2g) character with sizable contribution coming from the NCS ligands and the pi-bonding orbitals of the 4,4'-di-(2-(3,6-dimethoxyphenyl)ethenyl)-2,2'-bipyridine. The LUMO is a pi* orbital localized on the 4,4'-dicarboxylic acid-2,2'-bipyridine ligand. (c) 2006 Elsevier B.V. All rights reserved.
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