Gapless spin liquid of an organic triangular compound evidenced by thermodynamic measurements

In frustrated magnetic systems, long-range ordering is forbidden and degeneracy of energy states persists, even at extremely low temperatures. Under certain conditions, these systems form an exotic quantum spin-liquid ground state, in which strongly correlated spins fluctuate in the spin lattices. Here we investigate the thermodynamic properties of an anion radical spin liquid of EtMe3Sb[Pd(dmit)2]2, where dmit represents 1,3-dithiole-2-thione-4,5-dithiolate. This compound is an organic dimer-based Mott insulator with a two-dimensional triangular lattice structure. We present distinct evidence for the formation of a gapless spin liquid by examining the T-linear heat capacity coefficient, γ , in the low-temperature heat capacity. Using comparative analyses with κ-(BEDT-TTF)2Cu2(CN)3, a generalized picture of the new spin liquid in dimer-based organic systems is discussed. We also report anomalous enhancement of γ, produced by a kind of criticality inherent to the Pd(dmit)2 phase diagram. Frustrated magnetic systems can form an exotic quantum spin-liquid ground state, in which strongly correlated spins fluctuate in the spin lattices. Here, the low-temperature electronic state of a charge-transfer compound is found to form a gapless spin liquid.