Electron-electron interaction effects on the photophysics of metallic single-walled carbon nanotubes

Single-walled carbon nanotubes are strongly correlated systems with large Coulomb repulsion between two electrons occupying the same $p_z$ orbital. Within a molecular Hamiltonian appropriate for correlated $\pi$-electron systems, we show that optical excitations polarized parallel to the nanotube axes in the so-called metallic single-walled carbon nanotubes are to excitons. Our calculated absolute exciton energies in twelve different metallic single-walled carbon nanotubes, with diameters in the range 0.8 - 1.4 nm, are in nearly quantitative agreement with experimental results. We have also calculated the absorption spectrum for the (21,21) single-walled carbon nanotube in the E$_{22}$ region. Our calculated spectrum gives an excellent fit to the experimental absorption spectrum. In all cases our calculated exciton binding energies are only slightly smaller than those of semiconducting nanotubes with comparable diameters, in contradiction to results obtained within the {\it ab initio} approach, which predicts much smaller binding energies. We ascribe this difference to the difficulty of determining the behavior of systems with strong on-site Coulomb interactions within theories based on the density functional approach. As in the semiconducting nanotubes we predict in the metallic nanotubes a two-photon exciton above the lowest longitudinally polarized exciton that can be detected by ultrafast pump-probe spectroscopy. We also predict a subgap absorption polarized perpendicular to the nanotube axes below the lowest longitudinal exciton, blueshifted from the exact midgap by electron-electron interactions

Spin-Peierls Dimerization of a s=1/2 Heisenberg Antiferromagnet on a Square Lattice

Dimerization of a spin-half Heisenberg antiferromagnet on a square lattice is investigated for several possible dimerized configurations, some of which are shown to have lower ground state energies than the others. In particular, the lattice deformations resulting in alternate stronger and weaker couplings along both the principal axes of a square lattice are shown to result in a larger gain in magnetic energy. In addition, a `columnar' configuration is shown to have a lower ground state energy and a faster increase in the energy gap parameter than a `staggered' configuration. The inclusion of unexpanded exchange coupling leads to a power law behaviour for the magnetic energy gain and energy gap, which is qualitatively different from that reported earlier. Instead of increasing as $\delta ^{x}$, the two quantities depend on $\delta$ as $\delta ^{\nu}/| \ln \delta | .$ This is true both in the near critical regime $(0\leq \delta \leq 0.1)$ as well as in the far regime $(0\leq \delta <1)$. It is suggested that the unexpanded exchange coupling is as much a source of the logarithmic dependence as a correction due to the contribution of umklapp processes. Staggered magnetization is shown to follow the same $\delta$-dependence in all the configurations in the small $\delta$-regime, while for $0\leq \delta <1$, it follows the power law $\delta ^{x}$.Comment: 12 pages, 7 Postscript figures, RevTex forma

Excitons in quasi-one dimensional organics: Strong correlation approximation

An exciton theory for quasi-one dimensional organic materials is developed in the framework of the Su-Schrieffer-Heeger Hamiltonian augmented by short range extended Hubbard interactions. Within a strong electron-electron correlation approximation, the exciton properties are extensively studied. Using scattering theory, we analytically obtain the exciton energy and wavefunction and derive a criterion for the existence of a $B_u$ exciton. We also systematically investigate the effect of impurities on the coherent motion of an exciton. The coherence is measured by a suitably defined electron-hole correlation function. It is shown that, for impurities with an on-site potential, a crossover behavior will occur if the impurity strength is comparable to the bandwidth of the exciton, corresponding to exciton localization. For a charged impurity with a spatially extended potential, in addition to localization the exciton will dissociate into an uncorrelated electron-hole pair when the impurity is sufficiently strong to overcome the Coulomb interaction which binds the electron-hole pair. Interchain coupling effects are also discussed by considering two polymer chains coupled through nearest-neighbor interchain hopping $t_{\perp}$ and interchain Coulomb interaction $V_{\perp}$. Within the $t$ matrix scattering formalism, for every center-of-mass momentum, we find two poles determined only by $V_{\perp}$, which correspond to the interchain excitons. Finally, the exciton state is used to study the charge transfer from a polymer chain to an adjacent dopant molecule.Comment: 24 pages, 23 eps figures, pdf file of the paper availabl

Analytical solutions to the third-harmonic generation in trans-polyacetylene: Application of dipole-dipole correlation on the single electron models

The analytical solutions for the third-harmonic generation (THG) on infinite chains in both Su-Shrieffer-Heeger (SSH) and Takayama-Lin-Liu-Maki (TLM) models of trans-polyacetylene are obtained through the scheme of dipole-dipole ($DD$) correlation. They are not equivalent to the results obtained through static current-current ($J_0J_0$) correlation or under polarization operator $\hat{P}$. The van Hove singularity disappears exactly in the analytical forms, showing that the experimentally observed two-photon absorption peak (TPA) in THG may not be directly explained by the single electron models.Comment: 10 pages, 4 figures, submitted to Phys. Rev.

Nonlinear optical response and spin-charge separation in one-dimensional Mott insulators

We theoretically study the nonlinear optical response and photoexcited states of the Mott insulators. The nonlinear optical susceptibility \chi^(3) is calculated by using the exact diagonalization technique on small clusters. From the systematic study of the dependence of \chi^(3) on dimensionality, we find that the spin-charge separation plays a crucial role in enhancing \chi^(3) in the one-dimensional (1D) Mott insulators. Based on this result, we propose a holon-doublon model, which describes the nonlinear response in the 1D Mott insulators. These findings show that the spin-charge separation will become a key concept of optoelectronic devices.Comment: 5 pages with 3 figures, to appear in PRB RC, 15 August 200

Magnetic excitation spectrum of dimerized antiferromagnetic chains

Motivated by recent measurements on CuGeO$_3$ the spectrum of magnetic excitations of an antiferromagnetic $S=\frac{1}{2}$ chain with alternating coupling strength is investigated. Wave vector dependent magnons and a continuum with square root behavior at the band edges are found. The spectral density of the continua is calculated. Spin rotation symmetry fixes the gap of the continuum to be twice the elementary magnon gap. This is in excellent agreement with experimental results. In addition, the existence of bound states of two magnons is predicted: below the continuum a singlet and a triplet, above the continuum an ``anti-bound'' quintuplet. The results are based on field theoretic arguments, RPA calculations, and consideration of the limit of strong alternation.Comment: 4 pages, 4 figures included, Revte

Correlation Effect on Peierls Transition

The effect of correlation on Peierls transition, which is accompanied by a dimerization, t_d, of a bond alternation for transfer energy, has been examined for a half-filled one-dimensional electron system with on-site repulsive interaction (U). By applying the renormalization group method to the interaction of the bosonized Hamiltonian, the dimerization has been calculated variationally and self-consistently with a fixed electron-phonon coupling constant (\lambda) and it is shown that t_d takes a maximum as a function of U. The result is examined in terms of charge gap and spin gap and is compared with that of the numerical simulation by Hirsch [Phys. Rev. Lett 51 (1983) 296]. Relevance to the spin Peierls transition in organic conductors is discussed.Comment: 4 pages, 4 figures, to be published in J. Phys. Soc. Jpn. 71 No.3 (2002

Charge-Transfer Excitations in One-Dimensional Dimerized Mott Insulators

We investigate the optical properties of one-dimensional (1D) dimerized Mott insulators using the 1D dimerized extended Hubbard model. Numerical calculations and a perturbative analysis from the decoupled-dimer limit clarify that there are three relevant classes of charge-transfer (CT) states generated by photoexcitation: interdimer CT unbound states, interdimer CT exciton states, and intradimer CT exciton states. This classification is applied to understanding the optical properties of an organic molecular material, 1,3,5-trithia-2,4,6-triazapentalenyl (TTTA), which is known for its photoinduced transition from the dimerized spin-singlet phase to the regular paramagnetic phase. We conclude that the lowest photoexcited state of TTTA is the interdimer CT exciton state and the second lowest state is the intradimer CT exciton state.Comment: 6 pages, 6 figures, to be published in J. Phys. Soc. Jp

Electron correlation effects in electron-hole recombination in organic light-emitting diodes

We develop a general theory of electron--hole recombination in organic light emitting diodes that leads to formation of emissive singlet excitons and nonemissive triplet excitons. We briefly review other existing theories and show how our approach is substantively different from these theories. Using an exact time-dependent approach to the interchain/intermolecular charge-transfer within a long-range interacting model we find that, (i) the relative yield of the singlet exciton in polymers is considerably larger than the 25% predicted from statistical considerations, (ii) the singlet exciton yield increases with chain length in oligomers, and, (iii) in small molecules containing nitrogen heteroatoms, the relative yield of the singlet exciton is considerably smaller and may be even close to 25%. The above results are independent of whether or not the bond-charge repulsion, X_perp, is included in the interchain part of the Hamiltonian for the two-chain system. The larger (smaller) yield of the singlet (triplet) exciton in carbon-based long-chain polymers is a consequence of both its ionic (covalent) nature and smaller (larger) binding energy. In nitrogen containing monomers, wavefunctions are closer to the noninteracting limit, and this decreases (increases) the relative yield of the singlet (triplet) exciton. Our results are in qualitative agreement with electroluminescence experiments involving both molecular and polymeric light emitters. The time-dependent approach developed here for describing intermolecular charge-transfer processes is completely general and may be applied to many other such processes.Comment: 19 pages, 11 figure