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Register a new userOptical probe of carrier doping by X-ray irradiation in organic dimer Mott insulator $kappa$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}]$Cl
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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.
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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.
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.
We report X-ray irradiation-induced carrier doping effects on the electrical conductivity in the organic dimer-Mott insulators $kappa$-(ET)$_{2}$$X$ with $X =$ Cu[N(CN)$_{2}$]Cl and Cu$_{2}$(CN)$_{3}$. For $kappa$-(ET)$_{2}$Cu[N(CN)$_{2}$]Cl, we have observed a large decrease of the resistivity by 40 % with the irradiation at 300 K and the metal-like temperature dependence down to about 50 K. The irradiation-induced defects expected at the donor molecule sites might cause a local imbalance of the charge transfer in the crystal. Such molecular defects result in the effective doping of carriers into the half-filled dimer-Mott insulators.
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.
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.
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