A novel series of dipolar organic dyes containing diarylamine as the electron donor, 2-cyanoacrylic acid as the electron acceptor, and fluorene and a heteroaromatic ring as the conjugating bridge have been developed and characterized. These metal-free dyes exhibited very high molar extinction coefficients in the electronic absorption spectra and have been successfully fabricated as efficient nanocrystalline TiO2 dye-sensitized solar cells (DSSCs). The solar-energy-to-electricity conversion efficiencies of DSSCs ranged from 4.92 to 6.88 %, which reached 68–96 % of a standard device of N719 fabricated and measured under the same conditions. With a TiO2 film thickness of 6 μm, DSSCs based on these dyes had photocurrents surpassing that of the N719-based device. DFT computation results on these dyes also provide detailed structural information in connection with their high cell performance.
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