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Novel Pressure-Temperature Phase Diagram of Molecular Conductors Related to the High-Pressure Superconductor, β-Me4N[Pd(dmit)2]2

Abstract Dependence on cation size or terminal chalcogen atom X in the anion radical salts of Pd(dmiX)2 (X=S(t), Se(se)) with the tetrahedral cation Me4Z+ (Z=N, P, As and Sb) was investigated by resistivity measurements under high-pressure, X-ray crystal structure analyses and band calculations. At ambient pressure, these systems are considered to be a two-dimensional Mott insulator. β-Me4N[Pd(dmit)2]2 is a superconductor with T c=6.2 K at 6.5 kbar. In spite of very similar dimerized column structures, other compounds show very different temperature dependences of resistivity under pressure. The stability of the high-pressure metallic state is influenced by the dimensionality of the electronic structure at ambient pressure, which links to the degree of the dimerization.