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Register a new userCharge and spin interplay in a new spin liquid candidate BEDT-TTF-based organic Mott insulator
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Triangular lattice quasi-two-dimensional Mott insulators based on BEDT-TTF molecule and its analogies present the largest group of spin liquid candidates on triangular lattice. It was shown theoretically that spin liquid state in these materials can arize from a coupling to the fluctuating charge degree of freedom. In this work we discuss magnetic properties of one of such materials, $kappa$-(BEDT-TTF)$_2$Hg(SCN)$_2$Cl, which is known to be at the border of the phase transition from Mott insulator into a charge ordered state, and demonstrates charge order properties in the temperature range from 30 to 15~K. Our magnetic susceptibility and cantilever magnetisation measurements demonstrate an absence of spin order in this material down to 120~mK. We present arguments demonstrating that the charge order melting at low temperatures prevents ordering of spins.
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We have in detail characterized the anisotropic charge response of the dimer Mott insulator $kappa$-(BEDT-TTF)$_2$-Cu$_2$(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 $rho(T)$. 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 relaxor-like 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.
Geometrical frustration, quantum entanglement and disorder may prevent long-range order of localized spins with strong exchange interactions, resulting in a novel state of matter. $kappa$-(BEDT-TTF)$_2$-Cu$_2$(CN)$_3$ is considered the best approximation of this elusive quantum-spin-liquid state, but its ground-state properties remain puzzling. Here we present a multi-frequency electron-spin resonance study down to millikelvin temperatures, revealing a rapid drop of the spin susceptibility at $T^*=6,mathrm{K}$. This opening of a spin gap, accompanied by structural modifications, suggests the enigmatic `$6,mathrm{K}$-anomaly as the transition to a valence-bond-solid ground state. We identify an impurity contribution that becomes dominant when the intrinsic spins form singlets. Only probing the electrons directly manifests the pivotal role of defects for the low-energy properties of quantum-spin systems without magnetic order.
To elucidate the pressure evolution of the electronic structure in an antiferromagnetic dimer-Mott (DM) insulator ${beta}^{prime}$-(BEDT-TTF)$_2$ICl$_2$, which exhibits superconductivity at 14.2 K under 8 GPa, we measured the polarized infrared (IR) optical spectra under high pressure. At ambient pressure, two characteristic bands due to intra- and interdimer charge transfers have been observed in the IR spectra, supporting that this salt is a typical half-filled DM insulator at ambient pressure. With increasing pressure, however, the intradimer charge transfer excitation shifts to much lower energies, indicating that the effective electronic state changes from half-filled to 3/4-filled as a result of weakening of dimerization. This implies that the system approaches a charge-ordered state under high pressure, in which charge degrees of freedom emerge as an important factor. The present results suggest that charge fluctuation inside of dimers plays an important role in the high-temperature superconductivity.
Inelastic neutron scattering measurements on the molecular dimer-Mott insulator $kappa$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Cl reveal a phonon anomaly in a wide temperature range. Starting from $T_{rm ins}sim50$-$60$ K where the charge gap opens, the low-lying optical phonon modes become overdamped upon cooling towards the antiferromagnetic ordering temperature $T_mathrm{N} = 27$ K, where also a ferroelectric ordering at $T_{rm FE} approx T_{rm N}$ occurs. Conversely, the phonon damping becomes small again when spins and charges are ordered below $T_mathrm{N}$, while no change of the lattice symmetry is observed across $T_mathrm{N}$ in neutron diffraction measurements. We assign the phonon anomalies to structural fluctuations coupled to charge and spin degrees of freedom in the BEDT-TTF molecules.
Using a nonequilibrium implementation of the extended dynamical mean field theory (EDMFT) we simulate the relaxation after photo excitation in a strongly correlated electron system with antiferromagnetic spin interactions. We consider the $t$-$J$ model and focus on the interplay between the charge- and spin-dynamics in different excitation and doping regimes. The appearance of string states after a weak photo excitation manifests itself in a nontrivial scaling of the relaxation time with the exchange coupling and leads to a correlated oscillatory evolution of the kinetic energy and spin-spin correlation function. A strong excitation of the system, on the other hand, suppresses the spin correlations and results in a relaxation that is controlled by hole scattering. We discuss the possibility of detecting string states in optical and cold atom experiments.
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