Crystal stability and optical properties of organic chain compounds

The solution to the long-standing problem of the cohesion of organic chain compounds is proposed. We consider the tight-binding dielectric matrix with two electronic bands per chain, determine the corresponding hybridized collective modes, and show that three among them are considerably softened due to strong dipole-dipole and monopole-dipole interactions. By this we explain the unusual low-frequency optical activity of TTF-TCNQ, including the observed 10 meV anomaly. The softening of the modes also explains the cohesion of the mixed-stack lattice, the fractional charge transfer almost independent of the material, and the formation of the charged sheets in some compounds.