“…Furthermore, tunable optical properties by structural modulation make squaraine dyes more specific over the other metal-free organic dye architecture . Squaraine dyes have an inherent character to form highly aggregated structures on solid or metal oxide surfaces and in solutions, thus having a variety of applications. − Aggregation of dyes on the semiconducting TiO 2 surface is facile and known for diminishing the DSSC efficiency; ,, , however, squaraine dyes wrapped with alkyl groups control both the dye aggregation and charge recombination that enhances the device efficiency by boosting V OC and J SC . , Many skeletal changes have been done to the squaraine dyes apart from the donor–acceptor–donor architecture, which gave varying DSSC device efficiencies of 2.4–8.9%. ,,− Furthermore, the directions of pioneer studies on the photovoltaics are naturally oriented toward aqueous media. − DSSCs based on water showed relatively low device efficiency and require low pH of buffer solutions for the dye anchoring process; therefore, aqueous media were replaced immediately with organic solvents. ,, However, organic solvent-based electrolytes and additives are the reasons for high DSSC efficiency, but they are chemically hazardous, volatile, and inflammable, which limits their practical applications; therefore, nonhazardous electrolytes drew researchers’ attention once again toward water-based DSSCs. ,− Furthermore, aqueous DSSCs based on water electrolytic systems, dyes wrapped with alkyl groups to avoid dye desorption from TiO 2 , and the use of additives to prevent mass transport have been well explored to enhance the DSSC device efficiency. ,,,− Therefore, achieving a high device efficiency through 100% of water media is still a big task to accomplish . One of the challenges is tuning the charge transport property at the dye-TiO 2 /electrolyte interface, which is compatible with aqueous electrolytes.…”