Gapped magnetic ground state in the spin-liquid candidate κ-(BEDT-TTF)₂Ag₂(CN)₃ suggested by magnetic spectroscopy

Abstract

The nature of the magnetic ground state of highly frustrated systems remains puzzling to this day. Here, we have performed multifrequency electron spin resonance (ESR) measurements on a putative quantum spin liquid compound κ-(BEDT-TTF)₂Ag₂(CN)₃, which is a rare example of S=1/2 spins on a triangular lattice. At high temperatures, the spin susceptibility exhibits a weak temperature dependence which can be described by the Heisenberg model with an antiferromagnetic exchange interaction of strength J/kB≈175K. At low temperatures, however, the rapid drop of the static spin susceptibility, together with monotonic decrease of the ESR linewidth, indicates that strong singlet correlations develop below a pairing energy scale T∗ accompanied by a spin gap. On the other hand, a weak Curie-like spin susceptibility and the angular dependence of the linewidth suggest additional contributions from impurity spins. We propose the gradual formation of spin singlets with an inhomogeneous spin gap at low temperatures.