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Electrocrystallization of the bis(ethylenedithio)tetrathiafulvalene (BEDT-TTF) organic donor in the presence of the [Fe(ClCNAn) 3 ] 3- ris(chlorocyananilato)ferrate(III) paramagnetic anion in different stoichiometric ratios and solvent mixtures afforded two different hybrid systems formulated as [BEDT-TTF] 4 [Fe(ClCNAn) 3 ]·3H 2 O ( 1 ) and [BEDT-TTF] 5 [Fe(ClCNAn) 3 ] 2 ·2CH 3 CN ( 2 ) (An = anilato). Compounds 1 and 2 present unusual structures without the typical segregated organic and inorganic layers, where layers of 1 are formed by Λ and Δ enantiomers of the anionic paramagnetic complex together with mixed-valence BEDT-TTF tetramers, while layers of 2 are formed by Λ and Δ enantiomers of the paramagnetic complex together with dicationic BEDT-TTF dimers and monomers. Compounds 1 and 2 show semiconducting behaviors with room-temperature conductivities of ca. 6 × 10 -3 S cm -1 (ambient pressure) and 1 × 10 -3 S cm -1 (under applied pressure of 12.1 GPa), respectively, due to strong dimerization between the donors. Magnetic measurements performed on compound 1 indicate weak antiferromagnetic coupling between high-spin Fe III ( S  Fe = 5/2) and mixed-valence radical cation diyads (BEDT-TTF) 2  + ( S  rad = 1/2) mediated by the anilate ligands, together with an important Pauli paramagnetism typical for conducting systems.

Magnetic Molecular Conductors Based on Bis(ethylenedithio)tetrathiafulvalene (BEDT-TTF) and the Tris(chlorocyananilato)ferrate(III) Complex