Molecular Engineering of Anthracene Core-Based Hole-Transporting Materials for Organic and Perovskite Photovoltaics

[Image: see text] Anthracene core-based hole-transporting material containing TIPs (triisopropylsilylacetylene) has been spotlighted as potential donors for perovskite solar cells (SCs) due to their appropriate energy levels, efficient hole transport capacity, high stability, and high power conversion efficiency. Herein, we have efficiently designed seven new highly conjugated A–B–D–C–D molecules (AS1–AS7) containing an anthracene core. We used end-capped modifications of donor units with acceptor units on one side and then theoretically characterized them for their appropriate use for SC applications. Modern quantum chemistry techniques have theoretically described the R (reference molecule) and developed (AS1–AS7) molecules. Moreover, the proposed (AS1–AS7) molecules are explored with density functional theory (DFT) and time-dependent density functional theory (TD-DFT) employing B3LYP/6-31G(d,p), and numerous parameters like photovoltaic, optical and electronic characteristics, frontier molecular orbital, excitation, binding and reorganization (λ(e) and λ(h)) energies, open circuit voltage, light harvesting efficiency, transition density matrix, fill factor, and the density of states have been studied. End-capped modification causes a smaller band gap between the highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO), higher UV–vis absorption maxima, tuned energy levels, lower binding and reorganizational (λ(e) and λ(h)) energies, and larger V(oc) values in proposed (AS1–AS7) molecules than R. AS5 has a remarkable absorption maximum of 495.94 nm and a narrow optimal energy gap (E(g)) of 1.46 eV. Furthermore, a complex study of AS5:PC61BM has revealed extraordinary charge shifting at the HOMO (AS5)–LUMO (PC(61)BM) interface. Our results suggested that newly developed anthracene core-based compounds (AS1–AS7) would be effective candidates with excellent photovoltaic and optoelectronic properties and could be employed in future organic and perovskite SC applications.