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Radical cations of a heptathienoacene α,β‐substituted with four n‐decyl side groups (D4T7.+) form exceptionally stable π‐dimer dications already at ambient temperature (Chem. Comm. 2011, 47, 12622). This extraordinary π‐dimerization process is investigated here with a focus on the ultimate [D4T7.+]2 π‐dimer dication and yet‐unreported transitory species formed during and after the oxidation. To this...
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