Influence of terminal moiety on PCE of DSSCs: An In Silico study based on triazatruxene-benzothiadiazole dye

[Display omitted] •Photovoltaic and optical properties explored for ten novel dye molecules (ZA1-ZA10)•DFT (B3LYP/6-31G(d,p)) used to design ZA1-ZA10 via acceptor moiety modification.•ZA5 shows a significant absorption redshift to 1021 nm due to its acceptor moiety.•ZA1-ZA10/TiO2 complexes reveal anchoring potential and electron injection to TiO2.•The study aids solar cell advances through the precision molecular design of dyes. Our study utilized an experimentally synthesized dye as a reference molecule, employing a donor-π linker-acceptor (D-π-A) framework for organic solar cells. The molecule featured a triazatruxene group linked with alkyl branches as the donor and ethynyl benzoic acid as the acceptor, connected through a derivative of benzothiadiazole as the π linker. To improve optoelectronic and photovoltaic properties, ten theoretically designed dyes (ZA1–ZA10) are proposed, differing from the reference (R) by modifying the terminal acceptor moiety. Various quantum analyses, including frontier molecular orbitals, optical properties, reorganization energies, binding energies, transition density matrices (TDM), molecular electrostatic potential (MEP), dipole moment, and density of states were carried out at DFT/B3LYP/6-31G(d,p). Ground state geometries revealed a co-planar morphology in ZA1–ZA10, facilitating efficient charge transportation. TDM and MEP illustrated improved electronic transitions in the excited states. Computational analyses revealed superior photovoltaic properties of ZA1–ZA10. Notably, ZA5 exhibited the most significant redshift (1021 nm) in absorption, lowest bandgap (1.44 eV), smallest transition energy (1.21 eV), least binding energy (0.23 eV), and improved charge mobilities. Results from the adsorption of ZA1-ZA10 on the TiO2 layer confirmed their anchoring potential and effective injection of electrons to anatase (TiO2)9. These significant outcomes promise the potential and novelty of our designed dyes for higher power conversion efficiencies (PCE) in dye-sensitized solar cells (DSSCs).