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The Mott insulator kappa-(BEDT-TTF)2Cu[N(CN)2]Cl consists of molecular dimers arranged on an anisotropic triangular lattice and develops a canted antiferromagnetic ground state. It has recently been suggested that this system features purely electronic ferroelectricity which requires an electric dipole moment. Optical spectroscopy clearly rules out charge imbalance in this system, which excludes the existence of quantum electric dipoles on the dimers and subsequently a dipolar spin coupling. We suggest that the prominent in-plane dielectric response in kappa-(BEDT-TTF)2Cu[N(CN)2]Cl is due to short-range discommensurations of the antiferromagnetic phase in the temperature range 30 < T < 50 K, and domain wall relaxations at lower temperatures.
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The recently proposed multiferroic state of the charge-transfer salt {kappa}-(BEDT-TTF)$_2$Cu[N(CN)$_2$]Cl [P. Lunkenheimer et al., Nature Mater., vol. 11, pp. 755-758, Sept. 2012] has been studied by dc-conductivity, magnetic susceptibility and measurements of the dielectric constant on various, differently prepared single crystals. In the majority of crystals we confirm the existence of an order-disorder-type ferroelectric state which coincides with antiferromagnetic order. This phenomenology rules out scenarios which consider an inhomogeneous, short-range-ordered ferroelectric state. Measurements of the dielectric constant and the magnetic susceptibility on the same crystals reveal that both transitions lie very close to each other or even collapse, indicating that both types of order are intimately coupled to each other. We address issues of the frequency dependence of the dielectric constant {epsilon} and the dielectric loss {epsilon} and discuss sample-to-sample variations.
The interplane optical spectrum of the organic superconductor kappa-(BEDT-TTF)2Cu[N(CN)2]Br was investigated in the frequency range from 40 to 40,000 cm-1. The optical conductivity was obtained by Kramers-Kronig analysis of the reflectance. The absence of a Drude peak at low frequency is consistent with incoherent conductivity but in apparent contradiction to the metallic temperature dependence of the DC resistivity. We set an upper limit to the interplane transfer integral of tb = 0.1 meV. A model of defect-assisted interplane transport can account for this discrepancy. We also assign the phonon lines in the conductivity to the asymmetric modes of the ET molecule.
In the two-dimensional organic charge-transfer salts kappa-(BEDT-TTF)2Cu[N(CN)2]Br{x}Cl{1-x} a systematic variation of the Br content from x = 0 to 0.9 allows us to tune the Mott transition by increasing the bandwidth. At temperatures below 50 K, an energy gap develops in the Cl-rich samples and grows to approximately 1000 cm-1 for T -> 0. With increasing Br concentration spectral weight shifts into the gap region and eventually fills it up completely. As the samples with x = 0.73, 0.85 and 0.9 become metallic at low temperatures, a Drude-like response develops due to the coherent quasiparticles. Here, the quasiparticle scattering rate shows a omega^2 dependence and the effective mass of the carriers is enhanced in agreement with the predictions for a Fermi liquid. These typical signatures of strong electron-electron interactions are more pronounced for compositions close to the critical value x_c approx 0.7 where the metal-to-insulator transition occurs.
We study the role played by the magnetic frustration in the antiferromagnetic phase of the organic salt kappa-(BEDT-TTF)_ 2 Cu [N(CN)_2] Cl. Using the spatially anisotropic triangular Heisenberg model we analyze previous and new performed NMR experiments. We compute the 1/T_1 relaxation time by means of the modified spin wave theory. The strong suppression of the nuclear relaxation time observed experimentally under varying pressure and magnetic field is qualitatively well reproduced by the model. Our results suggest the existence of a close relation between the effects of pressure and magnetic frustration.
Static susceptibility of kappa-[(BEDT-TTF)1-x(BEDSe-TTF)x]2Cu[N(CN)2]Br alloys with the BEDSe-TTF content near the border-line of ambient pressure superconductivity (x~0.3) has been measured as a function of temperature, magnetic field, and pressure. A non-monotonic pressure dependence is observed for both the superconducting critical temperature and superconducting volume fraction, with both quantities showing growth under pressure in the initial pressure range P < 0.3 kbar. The results are discussed in comparison with the data on the related kappa-phase BEDT-TTF superconductors in which not a cation but anion sublattice is modified by alloying, namely the family kappa-(BEDT-TTF)2Cu[N(CN)2]Cl1-xBrx. PACS numbers: 74.62.Fj, 74.70.Kn.
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