Aniline and Indoline Donors Based Far‐Red Active Unsymmetrical Squaraine Dyes for Dye Sensitized Solar Cells

Abstract In dye‐sensitized solar cells (DSSC), controlling the dye‐aggregation on the metal‐oxide surface by appending the alkyl groups around the donor or π‐spacer unit of the dye is a potential approach to enhance DSSC efficiency. Further, rigidification of the dye structures by cyclization modulates the photophysical properties of the sensitizer. Here a series of donor‐acceptor‐donor (D‐A‐D) type far‐red active unsymmetrical squaraine dyes ( SQA ) have been designed and synthesized, where N,N‐dimethylaniline, methylated‐ and branched‐indoline have been used as donor units. These dyes showed absorption between 629–654 nm (λ max ) with the molar extinction coefficient of 1.49–1.94×10 5 M −1 cm −1 . Systematic enhancements in DSSC device efficiency have been observed due to the cyclization and alkyl‐groups incorporation in this set of dyes which were further enhanced with the addition of chenodeoxycholic acid (CDCA). The highest DSSC device efficiency of 4.78 % ( J sc of 8.77 mA/cm 2 and V oc of 692 mV) has been achieved for SQA3 . The IPCE profile of SQA dyes indicates the contribution of aggregated structures for the photocurrent generation. Further, co‐sensitization of SQA3 dye with a complementary visible light active dye AK4 showed the enhanced device efficiency of 6.27 % with panchromatic IPCE response.