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Register a new userTransport criticality of the first-order Mott transition in a quasi-two-dimensional organic conductor, $kappa$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Cl
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An organic Mott insulator, $kappa$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Cl, was investigated by resistance measurements under continuously controllable He gas pressure. The first-order Mott transition was demonstrated by observation of clear jump in the resistance variation against pressure. Its critical endpoint at 38 K is featured by vanishing of the resistive jump and critical divergence in pressure derivative of resistance, $|frac{1}{R}frac{partial R}{partial P}|$, which are consistent with the prediction of the dynamical mean field theory and have phenomenological correspondence with the liquid-gas transition. The present results provide the experimental basis for physics of the Mott transition criticality.
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The effect of disorder on the electronic properties near the Mott transition is studied in an organic superconductor $kappa$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Br, which is systematically irradiated by X-ray. We observe that X-ray irradiation causes Anderson-type electron localization due to molecular disorder. The resistivity at low temperatures demonstrates variable range hopping conduction with Coulomb interaction. The experimental results show clearly that the electron localization by disorder is enhanced by the Coulomb interaction near the Mott transition.
We investigated the infrared optical spectra of an organic dimer Mott insulator $kappa$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Cl, which was irradiated with X-rays. We observed that the irradiation caused a large spectral weight transfer from the mid-infrared region, where interband transitions in the dimer and Mott-Hubbard bands take place, to a Drude part in a low-energy region; this caused the Mott gap to collapse. The increase of the Drude part indicates a carrier doping into the Mott insulator due to irradiation defects. The strong redistribution of the spectral weight demonstrates that the organic Mott insulator is very close to the phase border of the bandwidth-controlled Mott transition.
The magnetic field effect on the phase diagram of the organic Mott system $kappa$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Br in which the bandwidth was tuned by the substitution of deuterated molecules was studied by means of the resistivity measurements performed in magnetic fields. The lower critical point of the first-order Mott transition, which ended on the upper critical field $H_{rm c2}$-temperature plane of the superconductivity, was determined experimentally in addition to the previously observed upper critical end point. The lower critical end point moved to a lower temperature with the suppression of $T_{rm c}$ in magnetic fields and the Mott transition recognized so far as the $S$-shaped curve reached $T =$ 0 when $H > H_{rm c2}$ in the end.
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.
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.
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