331 research outputs found
Stability of conductance oscillations in monatomic sodium wires
We study the stability of conductance oscillations in monatomic sodium wires
with respect to structural variations. The geometry, the electronic structure
and the electronic potential of sodium wires suspended between two sodium
electrodes are obtained from self-consistent density functional theory
calculations. The conductance is calculated within the framework of the
Landauer-B\"utttiker formalism, using the mode-matching technique as formulated
recently in a real-space finite-difference scheme [Phys. Rev. B \textbf{70},
195402 (2004)]. We find a regular even-odd conductance oscillation as a
function of the wire length, where wires comprising an odd number of atoms have
a conductance close to the quantum unit , and even-numbered
wires have a lower conductance. The conductance of odd-numbered wires is stable
with respect to geometry changes in the wire or in the contacts between the
wire and the electrodes; the conductance of even-numbered wires is more
sensitive. Geometry changes affect the spacing and widths of the wire
resonances. In the case of odd-numbered wires the transmission is on-resonance,
and hardly affected by the resonance shapes, whereas for even-numbered wires
the transmission is off-resonance and sensitive to the resonance shapes.
Predicting the amplitude of the conductance oscillation requires a
first-principles calculation based upon a realistic structure of the wire and
the leads. A simple tight-binding model is introduced to clarify these results.Comment: 16 pages, 20 figure
First principles modelling of magnesium titanium hydrides
Mixing Mg with Ti leads to a hydride Mg(x)Ti(1-x)H2 with markedly improved
(de)hydrogenation properties for x < 0.8, as compared to MgH2. Optically, thin
films of Mg(x)Ti(1-x)H2 have a black appearance, which is remarkable for a
hydride material. In this paper we study the structure and stability of
Mg(x)Ti(1-x)H2, x= 0-1 by first-principles calculations at the level of density
functional theory. We give evidence for a fluorite to rutile phase transition
at a critical composition x(c)= 0.8-0.9, which correlates with the
experimentally observed sharp decrease in (de)hydrogenation rates at this
composition. The densities of states of Mg(x)Ti(1-x)H2 have a peak at the Fermi
level, composed of Ti d states. Disorder in the positions of the Ti atoms
easily destroys the metallic plasma, however, which suppresses the optical
reflection. Interband transitions result in a featureless optical absorption
over a large energy range, causing the black appearance of Mg(x)Ti(1-x)H2.Comment: 22 pages, 9 figures, 4 table
Real space finite difference method for conductance calculations
We present a general method for calculating coherent electronic transport in
quantum wires and tunnel junctions. It is based upon a real space high order
finite difference representation of the single particle Hamiltonian and wave
functions. Landauer's formula is used to express the conductance as a
scattering problem. Dividing space into a scattering region and left and right
ideal electrode regions, this problem is solved by wave function matching (WFM)
in the boundary zones connecting these regions. The method is tested on a model
tunnel junction and applied to sodium atomic wires. In particular, we show that
using a high order finite difference approximation of the kinetic energy
operator leads to a high accuracy at moderate computational costs.Comment: 13 pages, 10 figure
Identification of a methylase required for 2-methylhopanoid production and implications for the interpretation of sedimentary hopanes
The rise of atmospheric oxygen has driven environmental change and biological evolution throughout much of Earth’s history and was enabled by the evolution of oxygenic photosynthesis in the cyanobacteria. Dating this metabolic innovation using inorganic proxies from sedimentary rocks has been difficult and one important approach has been to study the distributions of fossil lipids, such as steranes and 2-methylhopanes, as biomarkers for this process. 2-methylhopanes arise from degradation of 2-methylbacteriohopanepolyols (2-MeBHPs), lipids thought to be synthesized primarily by cyanobacteria. The discovery that 2-MeBHPs are produced by an anoxygenic phototroph, however, challenged both their taxonomic link with cyanobacteria and their functional link with oxygenic photosynthesis. Here, we identify a radical SAM methylase encoded by the hpnP gene that is required for methylation at the C-2 position in hopanoids. This gene is found in several, but not all, cyanobacteria and also in α -proteobacteria and acidobacteria. Thus, one cannot extrapolate from the presence of 2-methylhopanes alone, in modern environments or ancient sedimentary rocks, to a particular taxonomic group or metabolism. To understand the origin of this gene, we reconstructed the evolutionary history of HpnP. HpnP proteins from cyanobacteria, Methylobacterium species, and other α-proteobacteria form distinct phylogenetic clusters, but the branching order of these clades could not be confidently resolved. Hence,it is unclear whether HpnP, and 2-methylhopanoids, originated first in the cyanobacteria. In summary, existing evidence does not support the use of 2-methylhopanes as biomarkers for oxygenic photosynthesis
Ab-initio calculation of the electronic and optical excitations in polythiophene: effects of intra- and interchain screening
We present an calculation of the electronic and optical excitations of an
isolated polythiophene chain as well as of bulk polythiophene. We use the GW
approximation for the electronic self-energy and include excitonic effects by
solving the electron-hole Bethe-Salpeter equation. The inclusion of interchain
screening in the case of bulk polythiophene drastically reduces both the
quasi-particle band gap and the exciton binding energies, but the optical gap
is hardly affected. This finding is relevant for conjugated polymers in
general.Comment: 4 pages, 1 figur
Serum concentrations of the N-terminal propeptide of type III procollagen and two type IV collagen fragments and gene expression of the respective collagen types in liver in rats with dimethylnitrosamine-induced hepatic fibrosis
Paleoecology and paleoceanography of the Athel silicilyte, Ediacaran-Cambrian boundary, Sultanate of Oman
The Athel silicilyte is an enigmatic, hundreds of meters thick, finely laminated quartz deposit, in which silica precipitated in deep water (>~100–200 m) at the Ediacaran–Cambrian boundary in the South Oman Salt Basin. In contrast, Meso-Neoproterozoic sinks for marine silica were dominantly restricted to peritidal settings. The silicilyte is known to contain sterane biomarkers for demosponges, which today are benthic, obligately aerobic organisms. However, the basin has previously been described as permanently sulfidic and time-equivalent shallow-water carbonate platform and evaporitic facies lack silica. The Athel silicilyte thus represents a unique and poorly understood depositional system with implications for late Ediacaran marine chemistry and paleoecology. To address these issues, we made petrographic observations, analyzed biomarkers in the solvent-extractable bitumen, and measured whole-rock iron speciation and oxygen and silicon isotopes. These data indicate that the silicilyte is a distinct rock type both in its sedimentology and geochemistry and in the original biology present as compared to other facies from the same time period in Oman. The depositional environment of the silicilyte, as compared to the bounding shales, appears to have been more reducing at depth in sediments and possibly bottom waters with a significantly different biological community contributing to the preserved biomarkers. We propose a conceptual model for this system in which deeper, nutrient-rich waters mixed with surface seawater via episodic mixing, which stimulated primary production. The silica nucleated on this organic matter and then sank to the seafloor, forming the silicilyte in a sediment-starved system. We propose that the silicilyte may represent a type of environment that existed elsewhere during the Neoproterozoic. These environments may have represented an important locus for silica removal from the oceans
Ab-initio prediction of the electronic and optical excitations in polythiophene: isolated chains versus bulk polymer
We calculate the electronic and optical excitations of polythiophene using
the GW approximation for the electronic self-energy, and include excitonic
effects by solving the electron-hole Bethe-Salpeter equation. Two different
situations are studied: excitations on isolated chains and excitations on
chains in crystalline polythiophene. The dielectric tensor for the crystalline
situation is obtained by modeling the polymer chains as polarizable line
objects, with a long-wavelength polarizability tensor obtained from the
ab-initio polarizability function of the isolated chain. With this model
dielectric tensor we construct a screened interaction for the crystalline case,
including both intra- and interchain screening. In the crystalline situation
both the quasi-particle band gap and the exciton binding energies are
drastically reduced in comparison with the isolated chain. However, the optical
gap is hardly affected. We expect this result to be relevant for conjugated
polymers in general.Comment: 15 pages including 4 figures; to appear in Phys. Rev. B, 6/15/200
CaB_6: a new semiconducting material for spin electronics
Ferromagnetism was recently observed at unexpectedly high temperatures in
La-doped CaB_6. The starting point of all theoretical proposals to explain this
observation is a semimetallic electronic structure calculated for CaB_6 within
the local density approximation. Here we report the results of parameter-free
quasiparticle calculations of the single-particle excitation spectrum which
show that CaB_6 is not a semimetal but a semiconductor with a band gap of 0.8
eV. Magnetism in La_xCa_{1-x}B_6 occurs just on the metallic side of a Mott
transition in the La-induced impurity band.Comment: 4 pages, 1 postscript figur
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