Phase Competition and Superconductivity in $\hat{I}º$-(BEDT-TTF)${}_2$X: Importance of Intermolecular Coulomb Interactions

Abstract

We theoretically study the competition among different electronic phases in molecular conductors $\hat{I}º$-(BEDT-TTF)${}_2$X. The ground-state properties of a 3/4-filled extended Hubbard model with the $\hat{I}º$-type geometry are investigated by a variational Monte Carlo method. We find various competing phases: dimer-Mott insulator, polar charge-ordered insulator, 3-fold charge-ordered metal, and superconductivity, whose pairing symmetry is an "extended-$s$+$d_{x^2-y^2}$"-wave type. Our results show that the superconducting phase is stabilized not on the verge of the Mott metal-insulator transition but near charge order instabilities, clearly indicating the importance of the intradimer charge degree of freedom and the intermolecular Coulomb interactions, beyond the simple description of the half-filled Hubbard model.

5 pages, 4 figures + supplemental material