Thermodynamic Properties of κ-(BEDT-TTF)2X Salts: Electron Correlations and Superconductivity

Heat capacity measurements of κ-(BEDT-TTF)2X (BEDT-TTF: Bis(ethylendithio) tetrathiafulvalene, X: counteranions) which are classified as two-dimensional (2D) dimer-Mott system are reported. At first, we explain structural and electronic features originated from rigid dimerization in donor arrangement in 2D layers. The antiferromagnetic Mott insulating phase located at low-pressure region in the phase diagram shows vanishing γ electronic heat capacity coefficient in the heat capacity, which claims opening of a charge-gap in this insulating state. Then, a systematic change of the γ around the Mott boundary region is reported in relation to the glass freezing of ethylene dynamics. The thermodynamic parameters determined by ∆Cp/γTc of 10 K class superconductors, κ-(BEDT-TTF)2Cu(NCS)2 and κ-(BEDT-TTF)2Cu[N(CN)2]Br demonstrate that a rather large gap with a strong coupling character appears around the Fermi-surface. On the other hand, the low temperature heat capacity clearly shows a picture of nodal-gap structure due to an anisotropic pairing. The comparison with lower Tc compounds in the κ-type structure is also performed so as to discuss overall features of the κ-type superconductors. The heat capacity measurements of hole-doped systems containing mercury in the counteranions show an anomalous enhancement of γ, which is consistent with the T1−1 of NMR experiments etc. The results of heat capacity measurements under high pressures are also reported.