No Arabic abstract
We discuss the mechanism and the conditions for the appearance of synchronized charge oscillations which have been observed experimentally and theoretically after strong photoexcitation of dimerized systems. In the Hubbard model with on-site repulsion, the Bloch equations for a wave-number-dependent pseudospin -- whose components describe the charge-density difference, current density, and bond density between the two sublattices -- involve an alternatingly tilted pseudomagnetic field, which assists the synchronization of pseudospins with different wave numbers, irrespective of the initial condition. This fact is numerically confirmed by the dynamics in finite lattices based on the exact diagonalization method. In the presence of nearest-neighbor repulsion, however, the synchronization can be hindered by excitons. Therefore, the excitation of a sufficiently large density of free electron-hole pairs, but low density of excitons, is needed to achieve synchronization.
The synchronization of charge oscillations after photoexcitation that has been realized through the emergence of an electronic breathing mode on dimer lattices is studied here from the viewpoint of the competition between interactions and randomness. We employ an extended Hubbard model at three-quarter filling on a simple dimer lattice and add random numbers to all transfer integrals between nearest-neighbor sites. Photoinduced dynamics are calculated using the time-dependent Schrodinger equation by the exact diagonalization method. Although the randomness tends to unsynchronize charge oscillations on different bonds during and after photoexcitation, sufficiently strong on-site repulsion $U$ overcomes this effect and synchronizes these charge oscillations some time after strong photoexcitation. The degree of synchronization is evaluated using an order parameter that is derived from the time profiles of the current densities on all bonds. As to the nearest-neighbor interaction $V$, if $V$ is weakly attractive, it increases the order parameter by facilitating the charge oscillations. The relevance of these findings to previously reported experimental and theoretical results for the organic conductor $kappa$-(bis[ethylenedithio]tetrathiafulvalene)$_2$Cu[N(CN)$_2$]Br is discussed.
Photoinduced charge dynamics in dimerized systems is studied on the basis of the exact diagonalization method and the time-dependent Schrodinger equation for a one-dimensional spinless-fermion model at half filling and a two-dimensional model for $kappa$-(bis[ethylenedithio]tetrathiafulvalene)$_2$X [$kappa$-(BEDT-TTF)$_2$X] at three-quarter filling. After the application of a one-cycle pulse of a specifically polarized electric field, the charge densities at half of the sites of the system oscillate in the same phase and those at the other half oscillate in the opposite phase. For weak fields, the Fourier transform of the time profile of the charge density at any site after photoexcitation has peaks for finite-sized systems that correspond to those of the steady-state optical conductivity spectrum. For strong fields, these peaks are suppressed and a new peak appears on the high-energy side, that is, the charge densities mainly oscillate with a single frequency, although the oscillation is eventually damped. In the two-dimensional case without intersite repulsion and in the one-dimensional case, this frequency corresponds to charge-transfer processes by which all the bonds connecting the two classes of sites are exploited. Thus, this oscillation behaves as an electronic breathing mode. The relevance of the new peak to a recently found reflectivity peak in $kappa$-(BEDT-TTF)$_2$X after photoexcitation is discussed.
We study a model for the metal-insulator (MI) transition in the rare-earth nickelates RNiO$_3$, based upon a negative charge transfer energy and coupling to a rock-salt like lattice distortion of the NiO$_6$ octahedra. Using exact diagonalization and the Hartree-Fock approximation we demonstrate that electrons couple strongly to these distortions. For small distortions the system is metallic, with ground state of predominantly $d^8ligand$ character, where $ligand$ denotes a ligand hole. For sufficiently large distortions ($delta d_{rm Ni-O} sim 0.05 - 0.10AA$), however, a gap opens at the Fermi energy as the system enters a periodically distorted state alternating along the three crystallographic axes, with $(d^8ligand^2)_{S=0}(d^8)_{S=1}$ character, where $S$ is the total spin. Thus the MI transition may be viewed as being driven by an internal volume collapse where the NiO$_6$ octahedra with two ligand holes shrink around their central Ni, while the remaining octahedra expand accordingly, resulting in the ($1/2,1/2,1/2$) superstructure observed in x-ray diffraction in the insulating phase. This insulating state is an example of a new type of charge ordering achieved without any actual movement of the charge.
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.
Charge density wave, or CDW, is usually associated with Fermi surfaces nesting. We here report a new CDW mechanism discovered in a 2H-structured transition metal dichalcogenide, where the two essential ingredients of CDW are realized in very anomalous ways due to the strong-coupling nature of the electronic structure. Namely, the CDW gap is only partially open, and charge density wavevector match is fulfilled through participation of states of the large Fermi patch, while the straight FS sections have secondary or negligible contributions.