Unified understanding of superconductivity and Mott transition in alkali-doped fullerides from first principles

Abstract

Alkali-doped fullerides A3C60 (A=K, Rb, Cs) are surprising materials where conventional phonon-mediated superconductivity and unconventional Mott physics meet, leading to a remarkable phase diagram as a function of the volume per C60 molecule. Here we address these materials with a state-of-the-art calculation, where we construct a realistic low-energy model from first principles without using a priori information other than the crystal structure and solve it with an accurate many-body theory. Remarkably our scheme comprehensively reproduces the experimental phase diagram including the low-spin Mott-insulating phase next to the superconducting phase. Most remarkably, the critical temperature Tc's calculated from first principles quantitatively reproduce the experimental values. The driving force behind the surprising phase diagram of A3C60 is a subtle competition between Hund's coupling and Jahn-Teller phonons, which leads to an effectively inverted Hund's coupling. Our results establish that the fullerides are the first members of a novel class of molecular superconductors in which the multiorbital electronic correlations and phonons cooperate to reach high-Tc s-wave superconductivity.

Main text: 17 pages, 4 figures, 1 table. Supplemental Material: 9 pages, 2 figure, 2 tables

References in corpus (7)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• Modeling the Unconventional Superconducting Properties of Expanded A${}_3$C${}_{60}$ Fullerides
• Efficient DMFT-simulation of the Holstein-Hubbard Model
• Screening and Non-local Correlations in the Extended Hubbard Model from Self-Consistent Combined GW and Dynamical Mean Field Theory
• NMR study of the Mott transitions to superconductivity in the two Cs_3C_60 phases
• Superconductivity in the two-band Hubbard model
• Double-expansion impurity solver for multiorbital models with dynamically screened U and J

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