Self-Assembly of Rhenium(I) Double-Stranded Helicate and Mesocate from Flexible Ditopic Benzimidazolyl/Naphthanoimidazolyl N‑Donor and Rigid Bis-Chelating Hydroxyphenylbenzimidazolyl N∩OH-Donor Ligands: Synthesis, Characterization, and Photophysical and B‑DNA Docking Studies

The self-assembly of three rheniumtricarbonyl core-based supramolecular coordination complexes (SCCs), fac-[Re(CO)₃(μ-L)(μ-L′)Re(CO)₃] (1–3) was carried out using Re₂(CO)₁₀, rigid bis-chelating ligand (HO∩N-Ph-N∩OH (L¹) (where HO∩N = 2-hydroxyphenylbenzimidazolyl), and flexible ditopic N-donor ligands (L² = bis(3-((1H-benzoimidazol-1-yl)methyl)-2,4,6-trimethylphenyl)methane, L³ = bis(3-((1H-naphtho[2,3-d]imidazol-1-yl)methyl)-2,4,6-trimethylphenyl)methane, L⁴ = bis(4-(naphtho[2,3-d]imidazol-1-yl-methyl)phenyl)methane) via a one-pot solvothermal approach. In the solid state, the dinuclear SCCs adopt heteroleptic double-stranded helicate and meso-helicate architectures. The supramolecular structures of the complexes are retained in the solution based on the ¹H NMR and electrospray ionization (ESI)-mass analysis. The spectral and photophysical properties of the complexes were studied both experimentally and using time-dependent density functional theory (TDDFT) calculations. All of the supramolecules exhibited emission in both solution and solid states. Theoretical studies were conducted to determine the chemical reactivity parameters, molecular electrostatic potential surface plots, natural population, and Hirshfeld analysis for complexes 1–3. Additionally, molecular docking studies were carried out for complexes 1–3 with B-DNA.