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Three new electrochromic ferrocenyl triarylmethylium dyes with fluorenylium ( 1 a  + ,  1 b  + ) or thioxanthylium ( 1 c  + ) residues were selected in order to keep the intrinsic differences of redox potentials for ferrocene oxidation and triarylmethylium reduction small and to trigger valence tautomerism (VT). UV/Vis/NIR and quantitative EPR spectroscopy identified paramagnetic diradical isomers  1 a  ..+ – 1 c  ..+  alongside diamagnetic forms  1 a  + – 1 c  + , which renders these complexes magnetochemical switches. The diradical forms  1 a  ..+ – 1 c  ..+  as well as the one‐electron‐reduced triarylmethyl forms of the complexes were found to dimerize in solution. For radical  1 a  . , dimerization occurs on the timescale of cyclic voltammetry; this allowed us to determine the kinetics and equilibrium constant for this process by digital simulation. Mößbauer spectroscopy indicated that  1 a  +  and  1 b  +  retain VT even in the solid state. UV/Vis/NIR spectro‐electrochemistry revealed the poly‐electrochromic behaviour of these complexes by establishing the distinctly different electronic absorption profiles of the corresponding oxidized and reduced forms.

chemistry – a european journal

Tailoring Valence Tautomerism by Using Redox Potentials: Studies on Ferrocene‐Based Triarylmethylium Dyes with Electron‐Poor Fluorenylium and Thioxanthylium Acceptors