A new series of aromatic cyanovinyl compounds were synthesized via one-pot reactions of tri-or tetracyanoethylenes with nucleophilic reagents. The ground-state geometries and UV– vis absorption spectra of the compounds were computationally analyzed by means of density functional theory (DFT) and time-dependent density functional theory (TDDFT) calculations, respectively. None of the compounds were fluorescent in solution, but some ...