One-Electron Redox Reactions of Octamcthyl[4jradialene: Proof of the Alternancy of Even-Membered RadialenesThe photoelectron spectrum of octamethyl[4]radialene ( = tetrukis(dimethylmethy1idene)cyclobutune) yields the rather low first vertical ionization of only 7.30 eV and, therefore, the molecule can be oxidized by AICI,/CH,CI, to its radical cation. The ESR and ENDOR signal patterns recorded are almost identical with those of the radical anion, generated in a [2.2.2]cryptand THF solution by reduction at a potassium metal mirror. Their near congruency is in accord with the alternant rr molecular properties of even-membered radialenes as predicted by HMO theory, and larger changes of the D,, structure of C,(CH,), during the redox reactions are presumably hindered by the steric overcrowding in persubstituted [4]radialenes.