Intermolecular Coupling and Superconductivity in Chevrel Phase Compounds

To understand superconductivity in Chevrel phase compounds and guide the search for interesting properties in materials created with Chevrel phase molecules as building blocks, we use ab-initio methods to study the properties of single Mo6X8 molecules with X=S, Se, Te as well as the bulk solid PbMo6S8. In bulk PbMo6S8, the different energy scales from strong to weak are: the band kinetic energy, the intra-molecular Coulomb interaction, the on-molecule Jahn-Teller energy and the Hund's exchange coupling. The metallic state is stable with respect to Mott and polaronic insulating states. The bulk compound is characterized by a strong electron-phonon interaction with the largest coupling involving phonon modes with energies about 12 meV and with a strong inter-molecule (Peierls) character. A two-band Eliashberg equation analysis shows that the superconductivity has different gaps on the two Fermi surface sheets. A Bergman-Rainer analysis reveals that the Peierls modes provide the most important contribution to the superconductivity. This work illustrates the importance of inter-molecular coupling for collective phenomena in molecular solids.