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High-resolution photoemission study of metallic, insulating, and superconducting BEDT-TTF salts

A. Sekiyama, T. Susaki, A. Fujimori, T. Sasaki, N. Toyota, T. Kondo, G. Saito, M. Tsunekawa, T. Iwasaki, T. Muro, T. Matsushita, S. Suga, H. Ishii, T. Miyahara

DOI 10.1103/PhysRevB.56.9082 · Physical Review B

T1

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Abstract

We have made a high-resolution photoemission study of quasi-two-dimensional organic conductors BEDT-TTF salts which have various ground states, namely, antiferromagnetic insulator κ-(ET-d8)2Cu[N(CN)2]Cl, paramagnetic metal α-(ET)2KHg(SCN)4, and superconductors κ-(ET)2Cu(NCS)2 and κ -(ET)2Cu[N(CN)2]Br, where ET denotes BEDT-TTF or bisethylenedithio-tetrathiafulvalene. In all the spectra, the photoemission intensity is suppressed near the Fermi level (EF), especially for the κ-phase salts, although we have clearly observed a finite EF intensity for α-(ET)2KHg(SCN)4. Hartree-Fock band-structure calculations for the paramagnetic metallic and antiferromagnetic insulating states qualitatively explain the spectra of α-(ET)2KHg(SCN)4 and κ-(ET-d8)2Cu[N(CN)2]Cl, respectively, while those of κ-(ET)2Cu(NCS)2 and κ-(ET)2Cu[N(CN)2]Br strongly deviate from the calculations for the corresponding ground states. These observations imply that, among the metallic compounds, electrons are more strongly correlated in the κ-phase salts than in α-(ET)2KHg(SCN)4. It is shown that long-range electron correlation is quite important to explain the strong deviation of the spectra from the band-structure calculation. The spectra of the κ-phase salts exhibit a remarkable similarity between the metallic (superconducting) and insulating phases across the chemical pressure-induced phase transition. We have also observed unusual temperature dependence of the spectra for κ-(ET)2Cu(NCS)2, α-(ET)2KHg(SCN)4, and κ-(ET-d8)2Cu[N(CN)2]Cl.

Source-reported materials — not catalogue approval

FormulaReported Tc (K)Pressure (GPa)Type
κ-(ET)2Cu(NCS)2

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10Pressure not reportedunknown
κ-(ET)2Cu[N(CN)2]Br

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Source-occurrence policy only; no material identity or catalogue acceptance is inferred from the formula.

10Pressure not reportedunknown
κ-(ET)2Cu[N(CN)2]Cl

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Source-occurrence policy only; no material identity or catalogue acceptance is inferred from the formula.

—Pressure not reportedunknown

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