Novel cyano functional small molecule photosensitizers with amplified electron injection and photovoltaic attributes: molecular modelling towards efficient dye‐sensitized solar cells

Abstract BACKGROUND The exploration of novel photosensitizers with reverberant optoelectronic features for dye‐sensitized solar cells (DSSCs) is a frontline area of research. In this respect, attempts have been made to design a series of novel organic dyes (JFK‐1–JFK‐10) with D‐π‐A framework by π‐spacer modification strategy. The suitability of developed sensitizers for DSSCs applications is confirmed by executing natural bond orbital (NBO) analysis, transition density matrix (TDM) analysis, frontier molecular orbital (FMO) analysis, density of state (DOS) analysis, binding energy (Eb), electron regeneration energy (ΔGreg), free energy of injection (ΔGinject), electronic coupling constant (VRP), and intramolecular charge transfer (ICT) parameters qCT (e‐), DCT (Å), H index (Å), ∆(Å), t index (Å), μCT (D). RESULTS The calculated results of these analyses show that replacing the thiophene (B0) π‐spacer with extended conjugated thiazole and thiophene as a π‐spacer (B1‐B10) results in significantly lowered FMO energy levels, broader λ max values, and ICT parameters respectively. All the proposed dyes could be used as excellent sensitizers for DSSCs; the B9 spacer in JFK‐9 makes JFK‐9 a highly efficient candidate for the high‐efficiency of DSSCs due to promising photovoltaic characteristics, like the reduced Egap (4.386 eV), longer λ max (427.989 nm), longer excited state lifetimes (1.483 ns), a lower ΔGreg (1.807 eV), a greater dipole moment of (9.475 D), and large qCT (0.546), LHE (0.981), and eV OC (1.729 eV). CONCLUSION The fabricated dyes’ (F1‐F9) photoelectronic and chemical transfer parameters near the titania‐electrolyte interface (dyes@TiO 2 ) proved have better accumulation and recombination of dyes@TiO 2 model. The adsorption energies calculated of all compounds provide a deep insight into adsorption and charge transfer to a semiconductor TiO 2 conduction band. Hence, these modeled dyes (JFK‐1‐JFK‐10) could be used as efficient DSSCs and open new avenues for researchers to synthesize high‐performance DSSCs. © 2024 Society of Chemical Industry (SCI).