Substituent-Dependent Spin-Density Distribution and Coexistence of Fe 3d and π Spins on Ferrocene–Tetrathiafulvalene Hybrids

Ferrocene (Fc) and tetrathiafulvalene (TTF) moieties were incorporated into novel hybrid molecules of structure FcS4TTF­(R)2 (R = CF3 and SMe). [FcS4TTF­(R)2]•+ exhibited R-dependent spin-density distribution, and [FcS4TTF­(CF3)2]••2+ showed the coexistence of Fc-centered Fe 3d and TTF-centered π spins. The solid-state molecular structures in different oxidation states reflect their characteristic spin states.