C 13 NMR observation of a nonmagnetic charge-ordered state in the organic conductor κ − ( ET ) 2 Hg ( SCN ) 2 Cl

We investigated the local magnetism of the organic conductor, $κ$-(ET)$_{2}$Hg(SCN)$_{2}$Cl, with a quasi-triangular lattice of weakly dimerized molecules through $^{13}$C NMR spectroscopy. The NMR spectra and nuclear relaxation show that charge disproportionation occurs, associated with the metal-insulator transition at 31 K. The relaxation rate indicates that the paramagnetic spins in the insulating phase undergo a transition into a spin-singlet ground state with the emergence of orphan spins, a possible valence-bond-glass state. The present results are in high contrast to the spin-cluster paramagnetism of the electric dipole-liquid candidate, $κ$--(ET)$_{2}$Hg(SCN)$_{2}$Br, having nearly identical material parameters. This fact indicates that these two systems are on the verge between distinct phases in both charge and spin degrees of freedom; a spin-singlet charge-ordered state versus a spin-active Mott insulating state, competing with each other on a triangular lattice of dimerized sites.