Synthesis, Characterization, and DFT-Based Electronic and Nonlinear Optical Properties of Methyl 1-(arylsulfonyl)-2-aryl-1H-benzo[d]imidazole-6-carboxylates.

Herein, a series of N -1-sulfonyl substituted derivatives of 2-substituted benzimidazoles ( 2a - 2e ) were designed and synthesized via structural tailoring of the acceptor part of donor-π-acceptor schemes, and their nonlinear optic (NLO) characteristics were reported. The structures of 2a - 2e were investigated and their characterization was accomplished by employing spectroscopic procedures, i.e ., UV-vis, FT-IR, and 1 H and 13 C NMR. Further, a density functional theory (DFT) approach was used to calculate UV-vis, vibrational, and 1 H and 13 C NMR techniques; frontier molecular orbitals (FMOs); global reactivity parameters (GRPs); natural bond orbitals (NBOs); optical and vibrational analysis; and nonlinear optics (NLO). The most promising results were obtained for 6-nitro-2-(4-nitrophenyl)-1-(4-nitrophenylsulfonyl)-1 H -benzo[ d ]imidazole among entitled compounds, as it exhibited the highest ⟨α⟩ and β tot values, showing it is an eye-catching NLO material. This DFT study evokes the interest of researchers regarding the development of benzimidazole-based tempting NLO compounds that could be beneficial in modern hi-tech applications.