Thermodynamic properties of a spin-1/2 spin-liquid state in a κ-type organic salt

Abstract

In two-dimensional triangular lattices, geometric frustration prohibits the formation of ordering even at the lowest temperatures, and therefore a liquid-like ground state is expected. The spin-liquid problem has been one of the central topics of condensed-matter science for more than 30 yr in relation to the resonating-valence-bond model1. One of the characteristic features proposed is the existence of a linear temperature-dependent contribution to the heat capacity, as the degeneracy of the energy states should give rise to gapless excitations. Here, we show thermodynamic evidence for the realization of a spin-liquid ground state through a single-crystal calorimetric study of the dimer-based organic charge-transfer salt κ-(BEDT-TTF)2Cu2(CN)3, with a triangular lattice structure down to 75 mK. In addition, we report an unexpected hump structure in the heat capacity around 6 K, which may indicate a crossover into the quantum spin liquid.