Development of novel near-infrared (near-IR) dyes compatible with cobalt complex based redox shuttles for their utilization as sensitizer is inevitable for the fabrication of high-efficiency dye-sensitized solar cells (DSSCs). A series of newly designed unsymmetrical squaraine dyes as a model of near-IR sensitizer were synthesized and characterized for their application as far-red sensitizers of DSSCs utilizing Co(bpy)2+/3+ redox electrolyte. It was shown that logical molecular design led to not only energetic tunability of the sensitizers but also the possibility of good far-red photon harvesting up to 750 nm. One of the newly designed sensitizers, SQ-110, bearing two long alkyl substituents in combination with an electron donating methoxy group directly linked to the aromatic ring was par excellent in terms of its photoconversion efficiency among the dyes utilized in this work. DSSC fabricated using SQ-110 as sensitizer and Co(bpy)2+/3+ redox electrolyte furnished a photoconversion efficiency of 1.98% along with good photon harvesting mainly in the far-red wavelength region. It was further demonstrated that dye molecular structure plays a rather more prominent role than their energetics in controlling the overall device performance of the DSSCs.
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