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 (dmit2− = 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 λ-(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.