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The new heteroleptic ruthenium(II) complex containing a 1H-pyridin-(2E)-ylidene (PYE) ligand was synthesized and characterized using UV/Vis, FTIR, and NMR spectroscopies, mass spectrometry, elemental analysis, and cyclic voltammetry. The photovoltaic performance of the ruthenium complex as a charge transfer photosensitizer innc-titanium dioxide based dye-sensitized solar cell was studied and compared withcis-bis(isothiocyanato)(2,2′-bipyridyl-4,4′-dicarboxylato)(2,2′-bipyridyl-4,4′-di-nonyl)ruthenium(II) (Z907) under standard AM 1.5 sunlight. The complex CS90 gave a photocurrent density of 1.80 mA cm−2, 400 mV open-circuit potential, and 0.58 fill factor yielding an efficiency of 0.42% where the reference Z907 yielded an efficiency of 4.12%. The decrease in conversion efficiency observed for CS90 is attributed to a steric interaction between PYE and the TiO2surface that prevents optimum binding and also restricts ligand dynamics that are associated with oxidation state changes. [ABSTRACT FROM AUTHOR]