Interplay of conductivity, magnetism (and nonlinear optics) in organic-inorganic compounds

The preparation and characterization of organic-inorganic molecule-based systems in which conduction electrons coexist with localized moments is reported. These systems comprise (i) charge transfer salts of organic donors, such as BETS (bis(ethylenedithio)tetraselena-fulvalene and paramagnetic inorganic anions, such as [MX4](-), [M2X6](2-) with M = Fe, Cu, etc., and X = Cl, Br, etc., or (ii) charge transfer salts of inorganic acceptor bisdithiolato metal complexes, such as M(dmit)(2) (dmit(2-) = 2-thioxo-1,3-dithiole-4,5-dithiolato), and paramagnetic organometallic cations, such as [MCp2](n+) (Cp = cyclopentadienyl-like ligands). In some favorable cases, such as lambda-(BETS)(2)(FeCl4), new experimental evidence for interaction between the conduction electrons (of BETS) and magnetic moments (localized on [FeCl4](-)) is discussed. Current research towards the coupling of electrical and nonlinear optical properties in molecule-based compounds is reported. Additional evidence for the oxidation-induced symmetry breakdown in [bis-TTF](+) radical cations is given.