Unveiling the redox-active character of imidazolin-2-thiones derived from amino-substituted N-heterocyclic carbenes

IMes-derived thioureas in which the imidazolyl ring is directly substituted by one or two dimethylamino groups are redox-active, exhibiting one and two oxidized states, respectively. The structure, stability, and electronics of the oxidized species are investigated, emphasizing the decisive role of the amino substituents.