Triazatruxene Amine Donor-Based Visible-Light-Responsive Unsymmetrical Squaraine Dyes for Dye-Sensitized Solar Cells

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Optimized charge-transfer dynamics at the dye-TiO 2 /electrolyte interface are required for an enhanced dye-sensitized solar cell (DSSC) device performance. Such an optimized interface enhances the charge-injection, dye-regeneration, and diminished charge-recombination processes, synergistically enhancing the device efficiency. In this study, octupolar-structured sensitizers are designed to improve the interaction between the dye and the redox electrolyte for increasing the dye-regeneration process upon photoexcitation. Accordingly, a set of unsymmetrical squaraine dyes with indoline and triazatruxene amine donor-based D–A–D dyes are designed ( KV1 – KV3 ), synthesized, and sensitized with a semiconducting metal oxide (TiO 2 ) film. The sensitizer forms a monolayer on the TiO 2 surface, leading to a dye–dye interaction, which broadens the absorption spectrum. The N atom of the triazatruxene amine donor was left unsubstituted in KV1, whereas a hexyl chain was installed in KV2 and KV3 and a branched alkyl chain was installed on the core N atoms in KV3 to control the self-assembly of dyes on the TiO 2 surface. Self-assembly of alkyl groups wrapped in KV1 – KV3 dyes on the TiO 2 surface aids surface passivation and broadens the absorption profile, improving the light-harvesting capabilities. The DSSC devices based on KV2 exhibited a high power conversion efficiency of 7.85% ( V oc = 794 mV, J sc = 14.76 mA/cm 2, and FF = 67%), with an onset incident photon-to-current conversion efficiency response from 680 nm.