Anisotropic charge dynamics in the quantum spin-liquid candidate κ−(BEDT-TTF)2Cu2(CN)3

We have in detail characterized the anisotropic charge response of the dimer Mott insulator κ−(BEDT-TTF)2Cu2(CN)3 by dc conductivity, Hall effect, and dielectric spectroscopy. At room temperature, the Hall coefficient is positive and close to the value expected from stoichiometry; the temperature behavior follows the dc resistivity ρ(T). Within the planes the dc conductivity is well described by variable-range hopping in two dimensions; this model, however, fails for the out-of-plane direction. An unusually broad in-plane dielectric relaxation is detected below about 60 K; it slows down much faster than the dc conductivity following an Arrhenius law. At around 17 K, we can identify a pronounced dielectric anomaly concomitantly with anomalous features in the mean relaxation time and spectral broadening. The out-of-plane relaxation, on the other hand, shows a much weaker dielectric anomaly; it closely follows the temperature behavior of the respective dc resistivity. At lower temperatures, the dielectric constant becomes smaller both within and perpendicular to the planes; also, the relaxation levels off. The observed behavior bears features of relaxorlike ferroelectricity. Because heterogeneities impede its long-range development, only a weak-tunneling-like dynamics persists at low temperatures. We suggest that the random potential and domain structure gradually emerge due to the coupling to the anion network.