369 research outputs found
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 orbital.
Within a molecular Hamiltonian appropriate for correlated -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 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 , the two quantities depend on
as This is true both in the near critical
regime as well as in the far regime . 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 -dependence in all the configurations in the small -regime, while for
, it follows the power law .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 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 and interchain Coulomb interaction . Within the
matrix scattering formalism, for every center-of-mass momentum, we find two
poles determined only by , 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 ()
correlation. They are not equivalent to the results obtained through static
current-current () correlation or under polarization operator
. 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 the spectrum of magnetic
excitations of an antiferromagnetic 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
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