Search for high- Tc conventional superconductivity at megabar pressures in the lithium-sulfur system

Motivated by the recent report of superconductivity above 200 K in ultra-dense hydrogen sulfide, we search for high-TC conventional superconductivity in the phase diagram of the binary Li-S system, using ab initio methods for crystal structure prediction and linear response calculations for the electron-phonon coupling. We find that at pressures higher than 20 GPa, several new compositions, besides the known Li2S, are stabilized; many exhibit electride-like interstitial charge localization observed in other alkali-metal compounds. Of all predicted phases, only an fcc phase of Li3S, metastable before 640 GPa, exhibits a sizable TC, in contrast to what is observed in sulfur and phosphorus hydrides, where several stoichiometries lead to high TC. We attribute this difference to 2s−2phybridization and avoided core overlap, and predict similar behavior for other alkali-metal compounds.