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

[Image: see text] 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)-1H-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.