The metal-insulator transition in the organic conductor β^(primeprime)-(BEDT-TTF)₂Hg(SCN)₂Cl

We explore the nature of the metal-insulator transition in $\beta^{\prime\prime}$-(BEDT-TTF)$_{2}$Hg(SCN)$_{2}$Cl by x-ray, electrical transport, ESR, Raman and infrared investigations. Magnetic and vibrational spectroscopy concurrently reveal a gradual dimerization along the stacking direction $a$, setting in already at the crossover temperature of 150K from the metallic to the insulating state. A spin gap $\Delta_\sigma = 47$meV is extracted. From the activated resistivity behavior below 55K a charge gap $\Delta_\rho=60$meV is derived. At $T_{\rm CO} = 72$K the C=C vibrational modes reveal the development of a charge-ordered state with a charge disproportionation of $2\delta_{\rho}=0.34e$