582 research outputs found
Molecular structures and vibrations of neutral and anionic CuOx (x = 1-3,6) clusters
We report equilibrium geometric structures of CuO2, CuO3, CuO6, and CuO
clusters obtained by an all-electron linear combination of atomic orbitals
scheme within the density-functional theory with generalized gradient
approximation to describe the exchange-correlation effects. The vibrational
stability of all clusters is examined on the basis of the vibrational
frequencies. A structure with Cs symmetry is found to be the lowest-energy
structure for CuO2, while a -shaped structure with C2v symmetry is the most
stable structure for CuO3. For the larger CuO6 and CuO clusters, several
competitive structures exist with structures containing ozonide units being
higher in energy than those with O2 units. The infrared and Raman spectra are
calculated for the stable optimal geometries. ~Comment: Uses Revtex4, (Better quality figures can be obtained from authors
Density-functional-based predictions of Raman and IR spectra for small Si clusters
We have used a density-functional-based approach to study the response of silicon clusters to applied electric fields. For the dynamical response, we have calculated the Raman activities and infrared (IR) intensities for all of the vibrational modes of several clusters (SiN with N=3-8, 10, 13, 20, and 21) using the local density approximation (LDA). For the smaller clusters (N=3-8) our results are in good agreement with previous quantum-chemical calculations and experimental measurements, establishing that LDA-based IR and Raman data can be used in conjunction with measured spectra to determine the structure of clusters observed in experiment. To illustrate the potential of the method for larger clusters, we present calculated IR and Raman data for two low-energy isomers of Si10 and for the lowest-energy structure of Si13 found to date. For the static response, we compare our calculated polarizabilities for N=10, 13, 20, and 21 to recent experimental measurements. The calculated results are in rough agreement with experiment, but show less variation with cluster size than the measurements. Taken together, our results show that LDA calculations can offer a powerful means for establishing the structures of experimentally fabricated clusters and nanoscale systems
Magnetic isomers and local moment distribution in Mn5O and Mn6O clusters
A synergistic approach combining the experimental photoelectron spectroscopy and theoretical electronic structure studies is used to demonstrate the existence of magnetic isomers as well as configurations having comparable binding energies, identical spins, and yet differing in the distribution of local moments (called isomags). Our studies carried out on Mn5O and Mn6O clusters show that while the O atom occupies either bridge or hollow site with a binding energy of 6.88eV in Mn5, it prefers a hollow site with a binding energy of 7.18eV in Mn6 clusters. Mn5O is shown to possess two magnetic isomers with total spins of 13 and 5μB that contain three and five isomags, respectively. Mn6O possesses three isomers, two with moments of 8 and 2μBand a nonmagnetic. It is shown that the isomags, although undetected in magnetic experiments, can be identified via their electronic structure in experimental photoelectron spectra
Effect of local Coulomb interactions on the electronic structure and exchange interactions in Mn12 magnetic molecules
We have studied the effect of local Coulomb interactions on the electronic
structure of the molecular magnet Mn12-acetate within the LDA+U approach. The
account of the on-site repulsion results in a finite energy gap and an integer
value of the molecule's magnetic moment, both quantities being in a good
agreement with the experimental results. The resulting magnetic moments and
charge states of non-equivalent manganese ions agree very well with
experiments. The calculated values of the intramolecular exchange parameters
depend on the molecule's spin configuration, differing by 25-30% between the
ferrimagnetic ground state and the completely ferromagnetic configurations. The
values of the ground-state exchange coupling parameters are in reasonable
agreement with the recent data on the magnetization jumps in megagauss magnetic
fields. Simple estimates show that the obtained exchange parameters can be
applied, at least qualitatively, to the description of the spin excitations in
Mn12-acetate.Comment: RevTeX, LaTeX2e, 4 EPS figure
Theoretical Study of Cubic Structures Based on Fullerene Carbon Clusters: CC and (C
We study a new hypothetical form of solid carbon \csc, with a unit cell which
is composed of the \cs \ fullerene cluster and an additional single carbon atom
arranged in the zincblende structure. Using {\it ab initio} calculations, we
show that this new form of solid carbon has lower energy than hyperdiamond, the
recently proposed form composed of \cs \ units in the diamond structure. To
understand the bonding character of of these cluster-based solids, we analyze
the electronic structure of \csc \ and of hyperdiamond and compare them to the
electronic states of crystalline cubic diamond.Comment: 15 pages, latex, no figure
Importance of Correlation Effects on Magnetic Anisotropy in Fe and Ni
We calculate magnetic anisotropy energy of Fe and Ni by taking into account
the effects of strong electronic correlations, spin-orbit coupling, and
non-collinearity of intra-atomic magnetization. The LDA+U method is used and
its equivalence to dynamical mean-field theory in the static limit is
emphasized. Both experimental magnitude of MAE and direction of magnetization
are predicted correctly near U=4 eV for Ni and U=3.5 eV for Fe. Correlations
modify one-electron spectra which are now in better agreement with experiments.Comment: 4 pages, 2 figure
Metal-Insulator Transitions in Degenerate Hubbard Models and AC
Mott-Hubbard metal-insulator transitions in -fold degenerate Hubbard
models are studied within the Gutzwiller approximation. For any rational
filling with (integer) electrons per site it is found that metal-insulator
transition occurs at a critical correlation energy
, where
is the band energy per particle for the uncorrelated Fermi-liquid state and
is a geometric factor which increases linearly with . We
propose that the alkali metal doped fullerides can be described by
a 3-fold degenerate Hubbard model. Using the current estimate of band width and
correlation energy this implies that most of , at integer ,
are Mott-Hubbard insulators and is a strongly correlated
metal.Comment: 10 pages, Revte
Superconductivity in Fullerides
Experimental studies of superconductivity properties of fullerides are
briefly reviewed. Theoretical calculations of the electron-phonon coupling, in
particular for the intramolecular phonons, are discussed extensively. The
calculations are compared with coupling constants deduced from a number of
different experimental techniques. It is discussed why the A_3 C_60 are not
Mott-Hubbard insulators, in spite of the large Coulomb interaction. Estimates
of the Coulomb pseudopotential , describing the effect of the Coulomb
repulsion on the superconductivity, as well as possible electronic mechanisms
for the superconductivity are reviewed. The calculation of various properties
within the Migdal-Eliashberg theory and attempts to go beyond this theory are
described.Comment: 33 pages, latex2e, revtex using rmp style, 15 figures, submitted to
Review of Modern Physics, more information at
http://radix2.mpi-stuttgart.mpg.de/fullerene/fullerene.htm
Surface reconstruction induced geometries of Si clusters
We discuss a generalization of the surface reconstruction arguments for the
structure of intermediate size Si clusters, which leads to model geometries for
the sizes 33, 39 (two isomers), 45 (two isomers), 49 (two isomers), 57 and 61
(two isomers). The common feature in all these models is a structure that
closely resembles the most stable reconstruction of Si surfaces, surrounding a
core of bulk-like tetrahedrally bonded atoms. We investigate the energetics and
the electronic structure of these models through first-principles density
functional theory calculations. These models may be useful in understanding
experimental results on the reactivity of Si clusters and their shape as
inferred from mobility measurements.Comment: 9 figures (available from the author upon request) Submitted to Phys.
Rev.
Variations in the slope of the psychometric functions for speech intelligibility: a systematic survey
Although many studies have looked at the effects of different listening conditions on the intelligibility of speech, their analyses have often concentrated on changes to a single value on the psychometric function, namely, the threshold. Far less commonly has the slope of the psychometric function, that is, the rate at which intelligibility changes with level, been considered. The slope of the function is crucial because it is the slope, rather than the threshold, that determines the improvement in intelligibility caused by any given improvement in signal-to-noise ratio by, for instance, a hearing aid. The aim of the current study was to systematically survey and reanalyze the psychometric function data available in the literature in an attempt to quantify the range of slope changes across studies and to identify listening conditions that affect the slope of the psychometric function. The data for 885 individual psychometric functions, taken from 139 different studies, were fitted with a common logistic equation from which the slope was calculated. Large variations in slope across studies were found, with slope values ranging from as shallow as 1% per dB to as steep as 44% per dB (median = 6.6% per dB), suggesting that the perceptual benefit offered by an improvement in signal-to-noise ratio depends greatly on listening environment. The type and number of maskers used were found to be major factors on the value of the slope of the psychometric function while other minor effects of target predictability, target corpus, and target/masker similarity were also found
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