Dynamical study on polaron formation in a metal/polymer/metal structure

By considering a metal/polymer/metal structure within a tight-binding one-dimensional model, we have investigated the polaron formation in the presence of an electric field. When a sufficient voltage bias is applied to one of the metal electrodes, an electron is injected into the polymer chain, then a self-trapped polaron is formed at a few hundreds of femtoseconds while it moves slowly under a weak electric field (not larger than $$ V/cm). At an electric field between $1.0\times 10^4$ V/cm and $$ V/cm, the polaron is still formed, since the injected electron is bounded between the interface barriers for quite a long time. It is shown that the electric field applied at the polymer chain reduces effectively the potential barrier in the metal/polymer interface

Metal-insulator transition in the one-dimensional Holstein model at half filling

We study the one-dimensional Holstein model with spin-1/2 electrons at half-filling. Ground state properties are calculated for long chains with great accuracy using the density matrix renormalization group method and extrapolated to the thermodynamic limit. We show that for small electron-phonon coupling or large phonon frequency, the insulating Peierls ground state predicted by mean-field theory is destroyed by quantum lattice fluctuations and that the system remains in a metallic phase with a non-degenerate ground state and power-law electronic and phononic correlations. When the electron-phonon coupling becomes large or the phonon frequency small, the system undergoes a transition to an insulating Peierls phase with a two-fold degenerate ground state, long-range charge-density-wave order, a dimerized lattice structure, and a gap in the electronic excitation spectrum.Comment: 6 pages (LaTex), 10 eps figure

Peierls transition in the presence of finite-frequency phonons in the one-dimensional extended Peierls-Hubbard model at half-filling

We report quantum Monte Carlo (stochastic series expansion) results for the transition from a Mott insulator to a dimerized Peierls insulating state in a half-filled, 1D extended Hubbard model coupled to optical bond phonons. Using electron-electron (e-e) interaction parameters corresponding approximately to polyacetylene, we show that the Mott-Peierls transition occurs at a finite value of the electron-phonon (e-ph) coupling. We discuss several different criteria for detecting the transition and show that they give consistent results. We calculate the critical e-ph coupling as a function of the bare phonon frequency and also investigate the sensitivity of the critical coupling to the strength of the e-e interaction. In the limit of strong e-e couplings, we map the model to a spin-Peierls chain and compare the phase boundary with previous results for the spin-Peierls transition. We point out effects of a nonlinear spin-phonon coupling neglected in the mapping to the spin-Peierls model.Comment: 7 pages, 5 figure

Nonadiabatic approach to dimerization gap and optical absorption coefficient of the Su-Schrieffer-Heeger model

An analytical nonadiabatic approach has been developed to study the dimerization gap and the optical absorption coefficient of the Su-Schrieffer-Heeger model where the electrons interact with dispersive quantum phonons. By investigating quantitatively the effects of quantum phonon fluctuations on the gap order and the optical responses in this system, we show that the dimerization gap is much more reduced by the quantum lattice fluctuations than the optical absorption coefficient is. The calculated optical absorption coefficient and the density of states do not have the inverse-square-root singularity, but have a peak above the gap edge and there exist a significant tail below the peak. The peak of optical absorption spectrum is not directly corresponding to the dimerized gap. Our results of the optical absorption coefficient agree well with those of the experiments in both the shape and the peak position of the optical absorption spectrum.Comment: 14 pages, 7 figures. to be published in PR

Transition from band insulator to Mott insulator in one dimension: Critical behavior and phase diagram

We report a systematic study of the transition from a band insulator (BI) to a Mott insulator (MI) in a one-dimensional Hubbard model at half-filling with an on-site Coulomb interaction U and an alternating periodic site potential V. We employ both the zero-temperature density matrix renormalization group (DMRG) method to determine the gap and critical behavior of the system and the finite-temperature transfer matrix renormalization group method to evaluate the thermodynamic properties. We find two critical points at U = $U_c$ and U = $U_s$ that separate the BI and MI phases for a given V. A charge-neutral spin-singlet exciton band develops in the BI phase (U<$U_c$) and drops below the band gap when U exceeds a special point Ue. The exciton gap closes at the first critical point $U_c$ while the charge and spin gaps persist and coincide between $U_c$<U<$U_s$ where the system is dimerized. Both the charge and spin gaps collapse at U = $U_s$ when the transition to the MI phase occurs. In the MI phase (U>$U_s$) the charge gap increases almost linearly with U while the spin gap remains zero. These findings clarify earlier published results on the same model, and offer insights into several important issues regarding an appropriate scaling analysis of DMRG data and a full physical picture of the delicate nature of the phase transitions driven by electron correlation. The present work provides a comprehensive understanding for the critical behavior and phase diagram for the transition from BI to MI in one-dimensional correlated electron systems with a periodic alternating site potential.Comment: long version, 10 figure

Characterization of halogen-bridged binuclear metal complexes as hybridized two-band materials

We study the electronic structure of halogen-bridged binuclear metal (MMX) complexes with a two-band Peierls-Hubbard model. Based on a symmetry argument, various density-wave states are derived and characterized. The ground-state phase diagram is drawn within the Hartree-Fock approximation, while the thermal behavior is investigated using a quantum Monte Carlo method. All the calculations conclude that a typical MMX compound Pt_2(CH_3CS_2)_4I should indeed be regarded as a d-p-hybridized two-band material, where the oxidation of the halogen ions must be observed even in the ground state, whereas another MMX family (NH_4)_4[Pt_2(P_2O_5H_2)_4X] may be treated as single-band materials.Comment: 16 pages, 11 figures embedded, to be published in Phys. Rev.

Mean field approach to antiferromagnetic domains in the doped Hubbard model

We present a restricted path integral approach to the 2D and 3D repulsive Hubbard model. In this approach the partition function is approximated by restricting the summation over all states to a (small) subclass which is chosen such as to well represent the important states. This procedure generalizes mean field theory and can be systematically improved by including more states or fluctuations. We analyze in detail the simplest of these approximations which corresponds to summing over states with local antiferromagnetic (AF) order. If in the states considered the AF order changes sufficiently little in space and time, the path integral becomes a finite dimensional integral for which the saddle point evaluation is exact. This leads to generalized mean field equations allowing for the possibility of more than one relevant saddle points. In a big parameter regime (both in temperature and filling), we find that this integral has {\em two} relevant saddle points, one corresponding to finite AF order and the other without. These degenerate saddle points describe a phase of AF ordered fermions coexisting with free, metallic fermions. We argue that this mixed phase is a simple mean field description of a variety of possible inhomogeneous states, appropriate on length scales where these states appear homogeneous. We sketch systematic refinements of this approximation which can give more detailed descriptions of the system.Comment: 14 pages RevTex, 6 postscript figures included using eps

Landauer Theory, Inelastic Scattering and Electron Transport in Molecular Wires

In this paper we address the topic of inelastic electron scattering in mesoscopic quantum transport. For systems where only elastic scattering is present, Landauer theory provides an adequate description of transport that relates the electronic current to single-particle transmission and reflection probabilities. A formalism proposed recently by Bonca and Trugman facilitates the calculation of the one-electron transmission and reflection probabilities for inelastic processes in mesoscopic conductors connected to one-dimensional ideal leads. Building on their work, we have developed a self-consistent procedure for the evaluation of the non-equilibrium electron distributions in ideal leads connecting such mesoscopic conductors to electron reservoirs at finite temperatures and voltages. We evaluate the net electronic current flowing through the mesoscopic device by utilizing these non-equilibrium distributions. Our approach is a generalization of Landauer theory that takes account of the Pauli exclusion principle for the various competing elastic and inelastic processes while satisfying the requirement of particle conservation. As an application we examine the influence of elastic and inelastic scattering on conduction through a two site molecular wire with longitudinal phonons using the Su-Schrieffer-Heeger model of electron-phonon coupling.Comment: 25 pages, 8 figure

Polaron formation for a non-local electron-phonon coupling: A variational wave-function study

We introduce a variational wave-function to study the polaron formation when the electronic transfer integral depends on the relative displacement between nearest-neighbor sites giving rise to a non-local electron-phonon coupling with optical phonon modes. We analyze the ground state properties such as the energy, the electron-lattice correlation function, the phonon number and the spectral weight. Variational results are found in good agreement with analytic weak-coupling perturbative calculations and exact numerical diagonalization of small clusters. We determine the polaronic phase diagram and we find that the tendency towards strong localization is hindered from the pathological sign change of the effective next-nearest-neighbor hopping.Comment: 11 page

The low-lying excitations of polydiacetylene

The Pariser-Parr-Pople Hamiltonian is used to calculate and identify the nature of the low-lying vertical transition energies of polydiacetylene. The model is solved using the density matrix renormalisation group method for a fixed acetylenic geometry for chains of up to 102 atoms. The non-linear optical properties of polydiacetylene are considered, which are determined by the third-order susceptibility. The experimental 1Bu data of Giesa and Schultz are used as the geometric model for the calculation. For short chains, the calculated E(1Bu) agrees with the experimental value, within solvation effects (ca. 0.3 eV). The charge gap is used to characterise bound and unbound states. The nBu is above the charge gap and hence a continuum state; the 1Bu, 2Ag and mAg are not and hence are bound excitons. For large chain lengths, the nBu tends towards the charge gap as expected, strongly suggesting that the nBu is the conduction band edge. The conduction band edge for PDA is agreed in the literature to be ca. 3.0 eV. Accounting for the strong polarisation effects of the medium and polaron formation gives our calculated E(nBu) ca. 3.6 eV, with an exciton binding energy of ca. 1.0 eV. The 2Ag state is found to be above the 1Bu, which does not agree with relaxed transition experimental data. However, this could be resolved by including explicit lattice relaxation in the Pariser- Parr-Pople-Peierls model. Particle-hole separation data further suggest that the 1Bu, 2Ag and mAg are bound excitons, and that the nBu is an unbound exciton.Comment: LaTeX, 23 pages, 4 postscript tables and 8 postscript figure