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 ${\mathrm{Mo}}_6{X}_8$ molecules with $X=\text{S}$, Se, Te as well as the bulk solid ${\mathrm{PbMo}}_6{\mathrm{S}}_8$. In bulk ${\mathrm{PbMo}}_6{\mathrm{S}}_8$, the different energy scales from strong to weak are the band kinetic energy, the intramolecular 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 in the range from 11 to 17 meV and with a strong intermolecule (Peierls) character. A two-band Eliashberg equation analysis shows that the superconductivity is strong coupling, with different gaps on the two Fermi surface sheets. A Bergman-Rainer analysis of the functional derivative of the transition temperature with respect to the electron-phonon coupling reveals that the Peierls modes provide the most important contribution to the superconductivity. This work illustrates the importance of intermolecular coupling for collective phenomena in molecular solids.

• Received 18 September 2018

DOI:https://doi.org/10.1103/PhysRevMaterials.2.114801