Phase Transition in a One-Dimensional Extended Peierls-Hubbard Model with a Pulse of Oscillating Electric Field: III. Interference Caused by a Double Pulse

In order to study consequences of the differences between the ionic-to-neutral and neutral-to-ionic transitions in the one-dimensional extended Peierls-Hubbard model with alternating potentials for the TTF-CA complex, we introduce a double pulse of oscillating electric field in the time-dependent Schr\"odinger equation and vary the interval between the two pulses as well as their strengths. When the dimerized ionic phase is photoexcited, the interference effect is clearly observed owing to the coherence of charge density and lattice displacements. Namely, the two pulses constructively interfere with each other if the interval is a multiple of the period of the optical lattice vibration, while they destructively interfere if the interval is a half-odd integer times the period, in the processes toward the neutral phase. The interference is strong especially when the pulse is strong and short because the coherence is also strong. Meanwhile, when the neutral phase is photoexcited, the interference effect is almost invisible or weakly observed when the pulse is weak. The photoinduced lattice oscillations are incoherent due to random phases. The strength of the interference caused by a double pulse is a key quantity to distinguish the two transitions and to evaluate the coherence of charge density and lattice displacements.Comment: 16 pages, 8 figure

Charge ordering in \theta-(BEDT-TTF)2RbZn(SCN)4: Cooperative effects of electron correlations and lattice distortions

Combined effects of electron correlations and lattice distortions are investigated on the charge ordering in \theta-(BEDT-TTF)2RbZn(SCN)4 theoretically in a two-dimensional 3/4-filled extended Hubbard model with electron-lattice couplings. It is known that this material undergoes a phase transition from a high-symmetry metallic state to a low-symmetry insulating state with a horizontal-stripe charge order (CO) by lowering temperature. By means of the exact-diagonalization method, we show that electron-phonon interactions are crucial to stabilize the horizontal-stripe CO and to realize the low-symmetry crystal structure.Comment: 7 peges, 7 figures, accepted for publication in Phys. Rev.

Electron-Phonon Driven Spin Frustration in Multi-Band Hubbard Models: MX Chains and Oxide Superconductors

We discuss the consequences of both electron-phonon and electron-electron couplings in 1D and 2D multi-band (Peierls-Hubbard) models. After briefly discussing various analytic limits, we focus on (Hartree-Fock and exact) numerical studies in the intermediate regime for both couplings, where unusual spin-Peierls as well as long-period, frustrated ground states are found. Doping into such phases or near the phase boundaries can lead to further interesting phenomena such as separation of spin and charge, a dopant-induced phase transition of the global (parent) phase, or real-space (``bipolaronic'') pairing. We discuss possible experimentally observable consequences of this rich phase diagram for halogen-bridged, transition metal, linear chain complexes (MX chains) in 1D and the oxide superconductors in 2D.Comment: 6 pages, four postscript figures (appended), in regular Te

Phase Transition in a One-Dimensional Extended Peierls-Hubbard Model with a Pulse of Oscillating Electric Field: II. Linear Behavior in Neutral-to-Ionic Transition

Dynamics of charge density and lattice displacements after the neutral phase is photoexcited is studied by solving the time-dependent Schr\"odinger equation for a one-dimensional extended Peierls-Hubbard model with alternating potentials. In contrast to the ionic-to-neutral transition studied previously, the neutral-to-ionic transition proceeds in an uncooperative manner as far as the one-dimensional system is concerned. The final ionicity is a linear function of the increment of the total energy. After the electric field is turned off, the electronic state does not significantly change, roughly keeping the ionicity, even if the transition is not completed, because the ionic domains never proliferate. As a consequence, an electric field with frequency just at the linear absorption peak causes the neutral-to-ionic transition the most efficiently. These findings are consistent with the recent experiments on the mixed-stack organic charge-transfer complex, TTF-CA. We artificially modify or remove the electron-lattice coupling to discuss the origin of such differences between the two transitions.Comment: 17 pages, 9 figure

Nonequilibrium Green's-Function Approach to the Suppression of Rectification at Metal--Mott-Insulator Interfaces

Suppression of rectification at metal--Mott-insulator interfaces, which is previously shown by numerical solutions to the time-dependent Schr\"odinger equation and experiments on real devices, is reinvestigated theoretically by nonequilibrium Green's functions. The one-dimensional Hubbard model is used for a Mott insulator. The effects of attached metallic electrodes are incorporated into the self-energy. A scalar potential originating from work-function differences and satisfying the Poisson equation is added to the model. For the electron density, we decompose it into three parts. One is obtained by integrating the local density of states over energy to the midpoint of the electrodes' chemical potentials. The others, obtained by integrating lesser Green's functions, are due to the couplings with the electrodes and correspond to an inflow and an outflow of electrons. In Mott insulators, incoming electrons and holes are extended over the whole system, avoiding further accumulation of charge relative to the case without bias. This induces collective charge transport and results in the suppression of rectification.Comment: 18 pages, Figs. 1(b), 2, and 8 replaced. Corrected typo

Phase Transition in a One-Dimensional Extended Peierls-Hubbard Model with a Pulse of Oscillating Electric Field: I. Threshold Behavior in Ionic-to-Neutral Transition

Photoinduced dynamics of charge density and lattice displacements is calculated by solving the time-dependent Schr\"odinger equation for a one-dimensional extended Peierls-Hubbard model with alternating potentials for the mixed-stack organic charge-transfer complex, TTF-CA. A pulse of oscillating electric field is incorporated into the Peierls phase of the transfer integral. The frequency, the amplitude, and the duration of the pulse are varied to study the nonlinear and cooperative character of the photoinduced transition. When the dimerized ionic phase is photoexcited, the threshold behavior is clearly observed by plotting the final ionicity as a function of the increment of the total energy. Above the threshold photoexcitation, the electronic state reaches the neutral one with equidistant molecules after the electric field is turned off. The transition is initiated by nucleation of a metastable neutral domain, for which an electric field with frequency below the linear absorption peak is more effective than that at the peak. When the pulse is strong and short, the charge transfer takes place on the same time scale with the disappearance of dimerization. As the pulse becomes weak and long, the dimerization-induced polarization is disordered to restore the inversion symmetry on average before the charge transfer takes place to bring the system neutral. Thus, a paraelectric ionic phase is transiently realized by a weak electric field. It is shown that infrared light also induces the ionic-to-neutral transition, which is characterized by the threshold behavior.Comment: 24 pages, 11 figure

Spin-gap phase in nearly-half-filled one-dimensional conductors coupled with phonons

Asymptotic properties of nearly-half-filled one-dimensional conductors coupled with phonons are studied through a renormalization group method. Due to spin-charge coupling via electron-phonon interaction, the spin correlation varies with filling as well as the charge correlation. Depending on the relation between cut-off energy scales of the Umklapp process and of the electron-phonon interaction, various phases appear. We found a metallic phase with a spin gap and a dominant charge- density-wave correlation near half filling between a gapless density-wave phase (like in the doped repulsive Hubbard model) and a superconductor phase with a spin gap. The spin gap is produced by phonon-assisted backward scatterings which are interfered with the Umklapp process constructively or destructively depending on the character of electron-phonon coupling.Comment: 14 pages, revtex, replaced 5 ps figures, published in PR

Effects of Lattice and Molecular Phonons on Photoinduced Neutral-to-Ionic Transition Dynamics in Tetrathiafulvalene-pp-Chloranil

For electronic states and photoinduced charge dynamics near the neutral-ionic transition in the mixed-stack charge-transfer complex tetrathiafulvalene-$p$-chloranil (TTF-CA), we review the effects of Peierls coupling to lattice phonons modulating transfer integrals and Holstein couplings to molecular vibrations modulating site energies. The former stabilizes the ionic phase and reduces discontinuities in the phase transition, while the latter stabilizes the neutral phase and enhances the discontinuities. To reproduce the experimentally observed ionicity, optical conductivity and photoinduced charge dynamics, both couplings are quantitatively important. In particular, strong Holstein couplings to form the highly-stabilized neutral phase are necessary for the ionic phase to be a Mott insulator with large ionicity. A comparison with the observed photoinduced charge dynamics indicates the presence of strings of lattice dimerization in the neutral phase above the transition temperature.Comment: 9 pages, 7 figures, accepted for publication in J. Phys. Soc. Jp

Relaxation Dynamics of Photocarriers in One-Dimensional Mott Insulators Coupled to Phonons

We examine recombination processes of photocarriers in one-dimensional Mott insulators coupled to phonons. Performing density matrix renormalization group calculations, we find that, even for small electron-phonon coupling, many phonons are generated dynamically, which cause initial relaxation process after the irradiation. At the same time, spin-charge coupling coming from mixing of high- and low-energy states by the irradiation is suppressed. We discuss differences between Mott and band insulators in terms of relaxation dynamics.Comment: 5 pages, 3 figure