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Register a new userCollective excitation of electric dipole on molecular dimer in organic dimer-Mott insulator
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The terahertz (THz) response in 10-100 cm^-1 was investigated in an organic dimer-Mott (DM) insulator kappa-(ET)_2Cu_2(CN)_3 that exhibits a relaxor-like dielectric anomaly. 30 cm^-1 band in the optical conductivity was attributable to collective excitation of the intra-dimer electric dipoles which are formed by an electron correlation. We succeeded in observing photoinduced enhancement of this 30 cm^-1 band, reflecting the growth of the electric dipole cluster in the DM phase. Such optical responses in kappa-(ET)_2Cu_2(CN)_3 reflect instability near the boundary between the DM-ferroelectric charge ordered phases.
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We have observed the characteristic temperature dependence of the intermolecular phonon spectrum in the organic dimer Mott insulator kappa-(ET)2Cu2(CN)3 exhibiting a dielectric anomaly at 30 K. The anomalous spectral narrowing of the 55 cm-1 phonon peak at 30 K was analyzed in terms of motional narrowing within the framework of a stationary Gaussian process, i. e., the phonon frequency is modulated by the ultrafast charge fluctuation. The spectral narrowing occurs because the time constant of the correlation time tau_c and the amplitude of the frequency modulation delta satisfy the relation tau_c<delta at 30 K. At temperatures below 30 K, the motional narrowing is disturbed by the increasing of tau_c, near the charge-glass or the short-range order at 6 K. On the other hand, for temperatures above 30 K, the motional narrowing is disturbed by the increase of delta with increasing temperature.
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.
Magnetic excitation in a spin dimer system on a bilayer honeycomb lattice is investigated in the presence of a zigzag edge, where disordered and ordered phases can be controlled by a quantum phase transition. In analogy with the case of graphene with a zigzag edge, a flat edge magnon mode appears in the disordered phase. In an ordered phase, a finite magnetic moment generates a mean-field potential to the magnon. Since the potential is nonuniform on the edge and bulk sites, it affects the excitation, and the dispersion of the edge mode deviates from the flat shape. We investigate how the edge magnon mode evolves when the phase changes through the quantum phase transition and discuss the similarities to ordered spin systems on a monolayer honeycomb lattice.
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.
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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