Modeling the Unconventional Superconducting Properties of Expanded A$_3$C$_{60}$ Fullerides

TL;DR

This paper models the unconventional superconducting behavior of expanded A₃C₆₀ fullerides using a three-orbital Hubbard model and DMFT, revealing phenomena like pseudogaps and multiple energy scales that suggest strong correlations.

Contribution

It introduces a theoretical framework capturing the complex interplay of electron-electron and electron-phonon interactions in expanded fullerides, predicting unconventional properties.

Findings

Presence of a pseudogap in the normal phase

Increase in kinetic energy at superconducting transition

Multiple energy scales in single-particle dispersion

Abstract

The trivalent alkali fullerides A$_3$C$_{60}$, where C$_{60}$ are a well established family of molecular superconductors. The electron pairing has s-wave symmetry and is due to standard electron-phonon coupling, in particular by Jahn-Teller intramolecular C$_{60}$ vibrations. A source of renewed interest in these systems are indications of strong electron-electron repulsion, which emerges especially in compounds where the C$_{60}$-C$_{60}$ distance is expanded. In several compounds after an initial increases T$_c$, further expansions leads to a decline of superconductivity and its eventual disappearance in favor of a Mott insulating state We theoretically study a three-orbital Hubbard model including the phonon-mediated interaction using Dynamical Mean-Field Theory, which is particularly suitable due to the local nature of all the interactions. We studied the system as a function of the ratio of intra-molecular repulsion $U$ over the electron bandwidth $W$, the increase of $U/W$ representing the main effect of lattice expansion. The phase diagram is close to that of actual materials, with a dome-shaped superconducting region preceding the Mott transition. Unconventional properties predicted by this model include: (i) a pseudogap in the normal phase; (ii) a gain of kinetic energy and of d.c. conductivity at the onset of superconductivity; (iii) regular spin susceptibility and specific heat despite strong correlations; (iv) the emergence of more than one energy scale governing the renormalized single particle dispersion. These predictions, if confirmed, would establish fullerides, especially the expanded ones, as members of the wider family of strongly correlated superconductors.