Configurationally Stable Chiral Dithia‐Bridged Hetero[4]helicene Radical Cation: Electronic Structure and Absolute Configuration

Abstract A stable chiral hetero[4]helicene radical cation was synthesized and characterized by UV/Vis absorption and EPR spectroscopy, as well as X‐ray crystallography. For the first time, a combination of chiroptical methods involving ECD, ORD, and VCD, supported by quantum mechanical predictions, enabled the elucidation of the absolute configuration of such open‐shell helical species.