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Novel unsymmetrical organic sensitizers comprising donor, electron-conducting, and anchoring groups were engineered at a molecular level and synthesized for sensitization of mesoscopic titanium dioxide injection solar cells. The unsymmetrical organic sensitizers 3-(5-(4-(diphenylamino)styryl)thiophen-2-yl)-2-cyanoacrylic acid (D5), 3-(5-bis(4-(diphenylamino)styryl)thiophen-2-yl)-2-cyanoacrylic acid (D7), 5-(4-(bis(4-methoxyphenylamino)styryl)thiophen-2-yl)-2-cyanoacrylic acid (D9), and 3-(5-bis(4,4′-dimethoxydiphenylamino)styryl)thiophen-2-yl)-2-cyanoacrylic acid (D11) anchored onto TiO₂ and were tested in dye-sensitized solar cell with a volatile electrolyte. The monochromatic incident photon-to-current conversion efficiency of these sensitizers is above 80%, and D11-sensitized solar cells yield a short-circuit photocurrent density of 13.90 ± 0.2 mA/cm², an open-circuit voltage of 740 ± 10 mV, and a fill …