A. Islam, F. A. Chowdhury, Y. Chiba
Oct 6, 2006
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Chemistry of Materials
Abstract
A new series of aryl-substituted β-diketonato-ruthenium(II)-polypyridyl sensitizers, [Ru(Htctpy)(tfpbd)(NCS){(C4H9)4N}2] (1), [Ru(Htctpy)(tffpbd)(NCS){(C4H9)4N}2] (2), and [Ru(Htctpy)(tfcpbd)(NCS){(C4H9)4N}2] (3), were synthesized and fully characterized by elemental analysis, UV−visible and emission spectroscopy, NMR, ATR-FTIR, cyclic voltammetric studies, and density functional theory (DFT) calculations (where tctpy = 4,4‘4‘ ‘-tricarboxy-2,2‘:6‘,2‘ ‘-terpyridine, tfpbd = 4,4,4-trifluoro-1-(phenyl)butane-1,3-dione, tffpbd = 4,4,4-trifluoro-1- (4-fluorophenyl)butane-1,3-dione, and tfcpbd = 4,4,4-trifluoro-1-(4-chlorophenyl)butane-1,3-dione). In ethanol−methanol solution, these complexes exhibit intense visible light absorption, with low-energy MLCT band maxima above 600 nm. A distinct shoulder at around 680 nm improved red-light absorptivity beyond 680 nm. Controlled shifting of the low-energy MLCT band and Ru oxidation potential can be achieved by changing the electron donor ability of the β-diketonate l...