139 research outputs found
Thermodynamic perturbation theory for dipolar superparamagnets
Thermodynamic perturbation theory is employed to derive analytical
expressions for the equilibrium linear susceptibility and specific heat of
lattices of anisotropic classical spins weakly coupled by the dipole-dipole
interaction. The calculation is carried out to the second order in the coupling
constant over the temperature, while the single-spin anisotropy is treated
exactly. The temperature range of applicability of the results is, for weak
anisotropy (A/kT << 1), similar to that of ordinary high-temperature
expansions, but for moderately and strongly anisotropic spins (A/kT > 1) it can
extend down to the temperatures where the superparamagnetic blocking takes
place (A/kT \sim 25), provided only the interaction strength is weak enough.
Besides, taking exactly the anisotropy into account, the results describe as
particular cases the effects of the interactions on isotropic (A = 0) as well
as strongly anisotropic (A \to \infty) systems (discrete orientation model and
plane rotators).Comment: 15 pages, 3 figure
Prediction of infrared light emission from pi-conjugated polymers: a diagrammatic exciton basis valence bond theory
There is currently a great need for solid state lasers that emit in the
infrared, as this is the operating wavelength regime for applications in
telecommunications. Existing --conjugated polymers all emit in the visible
or ultraviolet, and whether or not --conjugated polymers that emit in the
infrared can be designed is an interesting challenge. On the one hand, the
excited state ordering in trans-polyacetylene, the --conjugated polymer
with relatively small optical gap, is not conducive to light emission because
of electron-electron interaction effects. On the other hand, excited state
ordering opposite to that in trans-polyacetylene is usually obtained by
chemical modification that increases the effective bond-alternation, which in
turn increases the optical gap. We develop a theory of electron correlation
effects in a model -conjugated polymer that is obtained by replacing the
hydrogen atoms of trans-polyacetylene with transverse conjugated groups, and
show that the effective on-site correlation in this system is smaller than the
bare correlation in the unsubstituted system. An optical gap in the infrared as
well as excited state ordering conducive to light emission is thereby predicted
upon similar structural modifications.Comment: 15 pages, 15 figures, 1 tabl
Spin Resolution of the Electron-Gas Correlation Energy: Positive same-spin contribution
The negative correlation energy per particle of a uniform electron gas of
density parameter and spin polarization is well known, but its
spin resolution into up-down, up-up, and down-down contributions is not.
Widely-used estimates are incorrect, and hamper the development of reliable
density functionals and pair distribution functions. For the spin resolution,
we present interpolations between high- and low-density limits that agree with
available Quantum Monte Carlo data. In the low-density limit for ,
we find that the same-spin correlation energy is unexpectedly positive, and we
explain why. We also estimate the up and down contributions to the kinetic
energy of correlation.Comment: new version, to appear in PRB Rapid Communicatio
Exchange Interaction in Binuclear Complexes with Rare Earth and Copper Ions: A Many-Body Model Study
We have used a many-body model Hamiltonian to study the nature of the
magnetic ground state of hetero-binuclear complexes involving rare-earth and
copper ions. We have taken into account all diagonal repulsions involving the
rare-earth 4f and 5d orbitals and the copper 3d orbital. Besides, we have
included direct exchange interaction, crystal field splitting of the rare-earth
atomic levels and spin-orbit interaction in the 4f orbitals. We have identified
the inter-orbital repulsion, U and crystal field parameter,
as the key parameters involved in controlling the type of exchange
interaction between the rare earth and copper 3d spins. We have explored
the nature of the ground state in the parameter space of U, ,
spin-orbit interaction strength and the filling n. We find
that these systems show low-spin or high-spin ground state depending on the
filling of the levels of the rare-earth ion and ground state spin is
critically dependent on U and . In case of half-filling
(Gd(III)) we find a reentrant low-spin state as U is increased, for
small values of , which explains the recently reported apparent
anomalous anti-ferromagnetic behaviour of Gd(III)-radical complexes. By varying
U we also observe a switch over in the ground state spin for other
fillings . We have introduced a spin-orbit coupling scheme which goes beyond
L-S or j-j coupling scheme and we find that spin-orbit coupling does not
significantly alter the basic picture.Comment: 22 pages, 11 ps figure
Theory of bound polarons in oxide compounds
We present a multilateral theoretical study of bound polarons in oxide
compounds MgO and \alpha-Al_2O_3 (corundum). A continuum theory at arbitrary
electron-phonon coupling is used for calculation of the energies of thermal
dissociation, photoionization (optically induced release of an electron (hole)
from the ground self-consistent state), as well as optical absorption to the
non-relaxed excited states. Unlike the case of free strong-coupling polarons,
where the ratio \kappa of the photoionization energy to the thermal
dissociation energy was shown to be always equal to 3, here this ratio depends
on the Froehlich coupling constant \alpha and the screened Coulomb interaction
strength \beta. Reasonable variation of these two parameters has demonstrated
that the magnitude of \kappa remains usually in the narrow interval from 1 to
2.5. This is in agreement with atomistic calculations and experimental data for
hole O^- polarons bound to the cation vacancy in MgO. The thermal dissociation
energy for the ground self-consistent state and the energy of the optically
induced charge transfer process (hops of a hole between O^{2-} ions) have been
calculated using the quantum-chemical method INDO. Results obtained within the
two approaches for hole O polarons bound by the cation vacancies (V^-) in
MgO and by the Mg^{2+} impurity (V_{Mg}) in corundum are compared to
experimental data and to each other. We discuss a surprising closeness of the
results obtained on the basis of independent models and their agreement with
experiment.Comment: 13 pages, 2 figures, 2 tables, E-mail addresses:
[email protected], [email protected]
Many-body-QED perturbation theory: Connection to the Bethe-Salpeter equation
The connection between many-body theory (MBPT)--in perturbative and
non-perturbative form--and quantum-electrodynamics (QED) is reviewed for
systems of two fermions in an external field. The treatment is mainly based
upon the recently developed covariant-evolution-operator method for QED
calculations [Lindgren et al. Phys. Rep. 389, 161 (2004)], which has a
structure quite akin to that of many-body perturbation theory. At the same time
this procedure is closely connected to the S-matrix and the Green's-function
formalisms and can therefore serve as a bridge between various approaches. It
is demonstrated that the MBPT-QED scheme, when carried to all orders, leads to
a Schroedinger-like equation, equivalent to the Bethe-Salpeter (BS) equation. A
Bloch equation in commutator form that can be used for an "extended" or
quasi-degenerate model space is derived. It has the same relation to the BS
equation as has the standard Bloch equation to the ordinary Schroedinger
equation and can be used to generate a perturbation expansion compatible with
the BS equation also for a quasi-degenerate model space.Comment: Submitted to Canadian J of Physic
Large scale numerical investigation of excited states in poly(phenylene)
A density matrix renormalisation group scheme is developed, allowing for the
first time essentially exact numerical solutions for the important excited
states of a realistic semi-empirical model for oligo-phenylenes. By monitoring
the evolution of the energies with chain length and comparing them to the
experimental absorption peaks of oligomers and thin films, we assign the four
characteristic absorption peaks of phenyl-based polymers. We also determine the
position and nature of the nonlinear optical states in this model.Comment: RevTeX, 10 pages, 4 eps figures included using eps
Formation and control of electron molecules in artificial atoms: Impurity and magnetic-field effects
Interelectron interactions and correlations in quantum dots can lead to
spontaneous symmetry breaking of the self-consistent mean field resulting in
formation of Wigner molecules. With the use of spin-and-space unrestricted
Hartree-Fock (sS-UHF) calculations, such symmetry breaking is discussed for
field-free conditions, as well as under the influence of an external magnetic
field. Using as paradigms impurity-doped (as well as the limiting case of
clean) two-electron quantum dots (which are analogs to helium-like atoms), it
is shown that the interplay between the interelectron repulsion and the
electronic zero-point kinetic energy leads, for a broad range of impurity
parameters, to formation of a singlet ground-state electron molecule,
reminiscent of the molecular picture of doubly-excited helium. Comparative
analysis of the conditional probability distributions for the sS-UHF and the
exact solutions for the ground state of two interacting electrons in a clean
parabolic quantum dot reveals that both of them describe formation of an
electron molecule with similar characteristics. The self-consistent field
associated with the triplet excited state of the two-electron quantum dot
(clean as well as impurity-doped) exhibits symmetry breaking of the Jahn-Teller
type, similar to that underlying formation of nonspherical open-shell nuclei
and metal clusters. Furthermore, impurity and/or magnetic-field effects can be
used to achieve controlled manipulation of the formation and pinning of the
discrete orientations of the Wigner molecules. Impurity effects are futher
illustrated for the case of a quantum dot with more than two electrons.Comment: Latex/Revtex, 10 pages with 4 gif figures. Small changes to explain
the difference between Wigner and Jahn-Teller electron molecules. A complete
version of the paper with high quality figures inside the text is available
at http://shale.physics.gatech.edu/~costas/qdhelium.html For related papers,
see http://www.prism.gatech.edu/~ph274c
Quasiparticle Density-Matrix Representation of Nonlinear TDDFT Response Functions
The time-dependent density functional (TDDFT) equations may be written either
for the Kohn-Sham orbitals in Hilbert space or for the single electron density
matrix in Liouville space. A collective-oscillator, quasiparticle,
representation of the density response of many-electron systems which
explicitly reveals the relevant electronic coherence sizes is developed using
the Liouville space representation of adiabatic TDDFT. Closed expressions for
the nonlinear density-density response are derived, eliminating the need to
solve nonlinear integral equations, as required in the Hilbert space
formulation of the response.Comment: 24 page
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