Supercritical fluid of quantum electrons in three-dimensional superconducting fullerides

Abstract

The supercritical fluid (SCF) of quantum electrons at the Mott metal-insulator transition without symmetry breaking is one of the most elusive phenomena in strongly correlated electron physics. Prior studies of Cr-doped V2O3 and organic Mott systems reported discrepant critical exponents. A key limitation is that the scaling analysis relies on a single experimental observable, leaving the roles of phase coexistence, inhomogeneity, and percolation unaddressed. Here we report the first experimental identification of a thermodynamically equilibrated SCF phase and its associated Mott endpoint in the three-dimensional superconducting fullerides CsxRb3-xC60, using two independent probes of electrical conductivity and magnetic susceptibility, which reveal two distinct metal-insulator transition lines converging at a single Mott endpoint. A hypothesis-free two-particle analysis of magnetic susceptibilities yields a metal-insulator coexisting SCF by exhibiting the maximum two-phase mixing entropy, in agreement with a picture of a thermodynamically equilibrated Widom line. Simultaneously, conductivity scaling yields a critical exponent in the regime of quantum critical predictions. Our new dual-probe approach provides a unified microscopic picture of the Mott SCF with a characteristic length scale below current diffraction resolution, in addition to a new interpretation on the origin of superconducting Tc-dome.