Abstract
The λ-type BETS conductors (BETS=bis(ethylenedithio)tetrathiafulvalene), λ-BETS 2MX 4 (M=Ga, Fe; X=C1, Br) afford an extremely large variety of low-temperature properties by substitution of metal (M) and halogen (X) atoms. In this paper the superconducting properties of λ-BETS 2GaBr x Cl 4− x and the coupling (or decoupling) of the antiferromagnetic and metal-insulator transitions of λ-BETS 2FeBr x Cl 4− x are reported. λ-BETS 2GaBr x Cl 4− x is an organic superconductor at x < 0.8. While λBETS 2GaBr 1.5Cl 2.5 is a semiconductor at ambient pressure and becomes a superconductor at high pressure. The maximum T c was almost the same as that of so-called “10 K-class organic superconductor” κ-ET 2Cu(NCS) 2. The anisotropic decrease of magnetic susceptibility of λ-BETS 2GaBr x Cl 4− x ( x > 1.0) suggested that non-antiferromagnetic insulating state is located near superconducting phase. The x-dependencies of resistivity and magnetic susceptibility of λ-BETS 2FeBr x Cl 4− x were also examined. At x < 0.2, the metal-insulator and antiferromagnetic transitions take place cooperatively. Around x=0.3, these two transitions tend to be separated At x > 0.6, the coupling between π and d electron systems becomes very weak and the Fe 3+ spins system undergoes an antiferromagnetic transition independently of π electron system. When the π-d coupling is strong ( x < 0.2), the magnetic easy axis of the antiferromagnetic structure is parallel to c. But it becomes perpendicular to c when the coupling becomes weak ( x > 0.6). The T-x phase diagrams of λ-BETS 2GaBr x Cl 4− x and λ-BETS 2FeBr x Cl 4− x resemble to each other. The superconducting phase of λBETS 2 GaBr x Cl 4− x appears at the x-region where the π-d coupling can be observed in λ-BETS 2FeBr x Cl 4− x .
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