Abstract

AbstractESR.‐spectra of the radical‐anions and the radical‐cations derived from two alkyl‐substituted, non‐alternant hydrocarbons, acepleiadiene (APH2) and 3,5,8,10‐tetramethyl‐cyclopenta[ef]heptalene (TMCP) have been recorded and analysed. The large differences in the total widths of the spectra of the corresponding ions (APH2⊖: 32; APH2⊕: 57; TMCP⊖: 69 and TMCP⊕: 36 Gauss) are well accounted for by the simple HMO model. The excellent agreement between the experimental and the theoretical values allows one to make a reliable assignment of the coupling constants to sets containing equal numbers of equivalent protons.

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