Thirty-Year Anniversary of <i>κ</i>-(BEDT-TTF)₂Cu₂(CN)₃: Reconciling the Spin Gap in a Spin-Liquid Candidate

Abstract

In 1991 the layered organic compound κ-(BEDT-TTF)2Cu2(CN)3 with a triangular lattice was synthesized for the first time. Although, originally, the focus was on the superconducting properties under pressure, this frustrated Mott insulator has been the most promising quantum-spin-liquid candidate for almost two decades, widely believed to host gapless spin excitations down to T→0. The recent observation of a spin gap rules out a gapless spin liquid with itinerant spinons and puts severe constraints on the magnetic ground state. This review evaluates magnetic, thermal transport, and structural anomalies around T⋆=6 K. The opening of a spin gap yields a rapid drop of spin susceptibility, NMR Knight shift, spin-lattice relaxation rate, and μ-SR spin fluctuation rate, but is often concealed by impurity spins. The concomitant structural transition at T⋆ manifests in thermal expansion, THz phonons and 63Cu NQR relaxation. Based on the field dependence of T⋆, a critical field of 30–60 T is estimated for the underlying spin-singlet state. Overall, the physical properties are remarkably similar to those of spin-Peierls compounds. Thus, a strong case is made that the ‘6K anomaly’ in κ-(BEDT-TTF)2Cu2(CN)3 is the transition to a valence-bond-solid state and it is suggested that such a scenario is rather the rule than the exception in materials with strong magnetic frustration.

Keywords

• charge-transfer salts
• (BEDT-TTF)₂<i>X</i>
• geometrical frustration
• quantum spin liquid
• valence bond solid
• strongly correlated electron systems