Electron Transfer and Exchange Interactions in Mixed-Valence Radical Anions, Radical Cations, and Neutral Diradicals Derived from Bridged Bis-Triarylmethyl Systems

| values. Complementary analyses of the MV anions and cations within the generalized Mulliken-Hush framework demonstrated effective CT coupling in both redox states. In each case, an energetically elevated CT state with bridge-centered charge localization strongly influenced the coupling. Frontier orbital analysis of hole and electron transfer clarified how donor- and acceptor-substitution modulates CT coupling. These results establish bridge electron density as a key parameter for tuning magnetic exchange and CT coupling, providing a basis for designing molecular architectures with controllable charge transport and magnetic properties.