Nonlinear optical response in doped conjugated polymers

Exciton effects on conjugated polymers are investigated in soliton lattice states. We use the Su-Schrieffer-Heeger model with long-range Coulomb interactions. The Hartree-Fock (HF) approximation and the single-excitation configuration- interaction (single-CI) method are used to obtain optical absorption spectra. The third-harmonic generation (THG) at off-resonant frequencies is calculated as functions of the soliton concentration and the chain length of the polymer. The magnitude of the THG at the 10 percent doping increases by the factor about 10^2 from that of the neutral system. This is owing to the accumulation of the oscillator strengths at the lowest exciton with increasing the soliton concentration. The increase by the order two is common for several choices of Coulomb interaction strengths.Comment: Accepted for publication in J. Phys.: Condens. Matte

Multi-Modes Phonon Softening in Two-Dimensional Electron-Lattice System

Phonon dispersion in a two-dimensional electron-lattice system described by a two-dimensional square-lattice version of Su-Schrieffer-Heeger's model and having the half-filled electronic band is studied theoretically at temperatures higher than the mean field critical temperature of the Peierls transition. When the temperature is lowered from the higher region down to the critical one, softening of multi phonon modes which have wave vectors equal to the nesting vector \vv{Q}=(\pi/a,\pi/a) with $a$ the lattice constant or parallel to \vv{Q} is observed. Although both of the transverse and longitudinal modes are softened at the critical temperature in the case of the wave vector equal to \vv{Q}, only the transverse modes are softened for other wave vectors parallel to \vv{Q}. This behavior is consistent with the Peierls distortions at lower temperatures.Comment: 10 pages, 5 Figure

Photogeneration Dynamics of a Soliton Pair in Polyacetylene

Dynamical process of the formation of a soliton pair from a photogenerated electron-hole pair in polyacetylene is studied numerically by adopting the SSH Hamiltonian. A weak local disorder is introduced in order to trigger the formation. Starting from an initial configuration with an electron at the bottom of the conduction band and a hole at the top of the valence band, separated by the Peierls gap, the time dependent Schr${\rm \ddot{o}}$ndinger equation for the electron wave functions and the equation of motion for the lattice displacements are solved numerically. After several uniform oscillations of the lattice system at the early stage, a large distortion corresponding to a pair of a soliton and an anti-soliton develops from a point which is determined by the location and type of the disorder. In some cases, two solitons run in opposite directions, leaving breather like oscillations behind, and in other cases they form a bound state emitting acoustic lattice vibrational modes.Comment: 16 pages 7 figure