Abstract A series of donor–π–acceptor systems incorporating a tetrathiafulvalene moiety as the donating unit have been designed and synthesized. The efficiency of the imine (–C= N–) bond as a conjugated π-linker in promoting intramolecular charge transfer is demonstrated and supported by calculations at the B3LYP/6-31G (d, p) level of theory. This property has been explored in the case of pyridyl-substituted systems which exhibit in particular a high ...