Conducting Molecular Magnets Based on TTF-Derivatives

The crystal structures, electronic and magnetic properties of conducting molecular magnets developed in our group are reviewed. (DMET)₂FeBr₄ is composed of alternating stacks of quasi-one-dimensional (1D) donor sheets and square lattice magnetic anion sheets. This salt undergoes an SDW transition of the donor layer at 40 K and an antiferromagnetic transition of Fe³⁺ spins on the anion layer at 3.7 K. The one-to-one correspondence of the anomalies appearing on the magnetization curves with those on the magnetoresistance supports the presence of the π-d interaction. (EDO-TTFI₂)₂M(mnt)₂] (M=Ni,Pt) consists of 1D chains of conducting donors and magnetic anions aligned in parallel. These salts show metallic conductivity accompanied with a metal-insulator transition around 90 K. Localized spins on the anions behave as a 1D ferromagnet, whose origin is explained by McConnell's first model. The properties of related materials, (EDTDM)₂FeBr₄, (EDS-TTF)₂FeBr₄ and (EDO-TTFBr₂)₂FeBr₄, are also presented.