137 research outputs found
Electrons in Dry DNA from Density Functional Calculations
The electronic structure of an infinite poly-guanine - poly-cytosine DNA
molecule in its dry A-helix structure is studied by means of density-functional
calculations. An extensive study of 30 nucleic base pairs is performed to
validate the method. The electronic energy bands of DNA close to the Fermi
level are then analyzed in order to clarify the electron transport properties
in this particularly simple DNA realization, probably the best suited candidate
for conduction. The energy scale found for the relevant band widths, as
compared with the energy fluctuations of vibrational or genetic-sequence
origin, makes highly implausible the coherent transport of electrons in this
system. The possibility of diffusive transport with sub-nanometer mean free
paths is, however, still open. Information for model Hamiltonians for
conduction is provided.Comment: 8 pages, 4 figure
Quasiparticle band structure of infinite hydrogen fluoride and hydrogen chloride chains
We study the quasiparticle band structure of isolated, infinite HF and HCl
bent (zigzag) chains and examine the effect of the crystal field on the energy
levels of the constituent monomers. The chains are one of the simplest but
realistic models of the corresponding three-dimensional crystalline solids. To
describe the isolated monomers and the chains, we set out from the Hartree-Fock
approximation, harnessing the advanced Green's function methods "local
molecular orbital algebraic diagrammatic construction" (ADC) scheme and "local
crystal orbital ADC" (CO-ADC) in a strict second order approximation, ADC(2,2)
and CO-ADC(2,2), respectively, to account for electron correlations. The
configuration space of the periodic correlation calculations is found to
converge rapidly only requiring nearest-neighbor contributions to be regarded.
Although electron correlations cause a pronounced shift of the quasiparticle
band structure of the chains with respect to the Hartree-Fock result, the
bandwidth essentially remains unaltered in contrast to, e.g., covalently bound
compounds.Comment: 11 pages, 6 figures, 6 tables, RevTeX4, corrected typoe
Ab initio Green's function formalism for band structures
Using the Green's function formalism, an ab initio theory for band structures
of crystals is derived starting from the Hartree-Fock approximation. It is
based on the algebraic diagrammatic construction scheme for the self-energy
which is formulated for crystal orbitals (CO-ADC). In this approach, the poles
of the Green's function are determined by solving a suitable Hermitian
eigenvalue problem. The method is not only applicable to the outer valence and
conduction bands, it is also stable for inner valence bands where strong
electron correlations are effective. The key to the proposed scheme is to
evaluate the self-energy in terms of Wannier orbitals before transforming it to
a crystal momentum representation. Exploiting the fact that electron
correlations are mainly local, one can truncate the lattice summations by an
appropriate configuration selection scheme. This yields a flat configuration
space; i.e., its size scales only linearly with the number of atoms per unit
cell for large systems and, under certain conditions, the computational effort
to determine band structures also scales linearly. As a first application of
the new formalism, a lithium fluoride crystal has been chosen. A minimal basis
set description is studied, and a satisfactory agreement with previous
theoretical and experimental results for the fundamental band gap and the width
of the F 2p valence band complex is obtained.Comment: 20 pages, 3 figures, 1 table, RevTeX4, new section on lithium
fluorid
What one can expect from the research performed on highly conducting polymers
449-452In this introductory paper the practical importance of the experimental and theoretical research on highly conducting polymers is considered. Further, the results of ab initio Hartree-Fock crystal orbital calculations (in some cases corrected also for correlation) on doped and on highly conducting polymers with small gaps (possibility of intrinsic conduction) are reviewed. The theoretical possibilities of improving these band structure calculations to a great extent (good basis set + correlation corrections) due to recent developments in programming are outlined. Finally, the possibilities of using these improved band structures for calculation of electron-phonon interactions (mobility) for soliton and bipolaron studies in these systems and for computing their Auger- and exciton spectra are pointed out. It is concluded that these theoretical developments will lead, within a few years, to the design of new highly conducting polymers with other optimal physical properties ("tailor made polymers") which are necessary to increase their practical applicability to a large extent
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