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Register a new userPhonon-Spectrum Narrowing Induced by Ultrafast Charge Fluctuation in an Organic Dimer Mott Insulator
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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.
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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.
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.
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.
Femtosecond time-resolved core-level photoemission spectroscopy with a free-electron laser is used to measure the atomic-site specific charge-order dynamics in the charge-density-wave/Mott insulator 1T-TaS2. After strong photoexcitation, a prompt loss of charge order and subsequent fast equilibration dynamics of the electron-lattice system are observed. On the time scale of electron-phonon thermalization, about 1 ps, the system is driven across a phase transition from a long-range charge ordered state to a quasi-equilibrium state with domain-like short-range charge and lattice order. The experiment opens the way to study the nonequilibrium dynamics of condensed matter systems with full elemental, chemical, and atomic site selectivity.
We use midinfrared pulses with stable carrier-envelope phase offset to drive molecular vibrations in the charge transfer salt ET-F2TCNQ, a prototypical one-dimensional Mott insulator. We find that the Mott gap, which is probed resonantly with 10 fs laser pulses, oscillates with the pump field. This observation reveals that molecular excitations can coherently perturb the electronic on-site interactions (Hubbard U) by changing the local orbital wave function. The gap oscillates at twice the frequency of the vibrational mode, indicating that the molecular distortions couple quadratically to the local charge density.
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