1,550 research outputs found
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
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
Investigation of the Jahn-Teller Transition in TiF3 using Density Functional Theory
We use first principles density functional theory to calculate electronic and
magnetic properties of TiF3 using the full potential linearized augmented plane
wave method. The LDA approximation predicts a fully saturated ferromagnetic
metal and finds degenerate energy minima for high and low symmetry structures.
The experimentally observed Jahn-Teller phase transition at Tc=370K can not be
driven by the electron-phonon interaction alone, which is usually described
accurately by LDA.
Electron correlations beyond LDA are essential to lift the degeneracy of the
singly occupied Ti t2g orbital. Although the on-site Coulomb correlations are
important, the direction of the t2g-level splitting is determined by the
dipole-dipole interactions. The LDA+U functional predicts an aniferromagnetic
insulator with an orbitally ordered ground state. The input parameters U=8.1 eV
and J=0.9 eV for the Ti 3d orbital were found by varying the total charge on
the TiF ion using the molecular NRLMOL code. We estimate the
Heisenberg exchange constant for spin-1/2 on a cubic lattice to be
approximately 24 K. The symmetry lowering energy in LDA+U is about 900 K per
TiF3 formula unit.Comment: 7 pages, 9 figures, to appear in Phys. Rev.
Low energy magnetic excitations of the Mn_{12}-acetate spin cluster observed by neutron scattering
We performed high resolution diffraction and inelastic neutron scattering
measurements of Mn_{12}-acetate. Using a very high energy resolution, we could
separate the energy levels corresponding to the splitting of the lowest S
multiplet. Data were analyzed within a single spin model (S=10 ground state),
using a spin Hamiltonian with parameters up to 4^{th} order.
The non regular spacing of the transition energies unambiguously shows the
presence of high order terms in the anisotropy (D= -0.457(2) cm^{-1}, B_4^0 =
-2.33(4) 10^{-5}cm^{-1}).
The relative intensity of the lowest energy peaks is very sensitive to the
small transverse term, supposed to be mainly responsible for quantum tunneling.
This allows an accurate determination of this term in zero magnetic field
(B_4^4 = \pm 3.0(5) 10^{-5} cm^{-1}). The neutron results are discussed in view
of recent experiments and theories.Comment: 4 pages ? 3 figures, submitted to Physical Review Lette
A critical assessment of the Self-Interaction Corrected Local Density Functional method and its algorithmic implementation
We calculate the electronic structure of several atoms and small molecules by
direct minimization of the Self-Interaction Corrected Local Density
Approximation (SIC-LDA) functional. To do this we first derive an expression
for the gradient of this functional under the constraint that the orbitals be
orthogonal and show that previously given expressions do not correctly
incorporate this constraint. In our atomic calculations the SIC-LDA yields
total energies, ionization energies and charge densities that are superior to
results obtained with the Local Density Approximation (LDA). However, for
molecules SIC-LDA gives bond lengths and reaction energies that are inferior to
those obtained from LDA. The nonlocal BLYP functional, which we include as a
representative GGA functional, outperforms both LDA and SIC-LDA for all ground
state properties we considered.Comment: 14 pages, 5 figure
Variational Hilbert space truncation approach to quantum Heisenberg antiferromagnets on frustrated clusters
We study the spin- Heisenberg antiferromagnet on a series of
finite-size clusters with features inspired by the fullerenes. Frustration due
to the presence of pentagonal rings makes such structures challenging in the
context of quantum Monte-Carlo methods. We use an exact diagonalization
approach combined with a truncation method in which only the most important
basis states of the Hilbert space are retained. We describe an efficient
variational method for finding an optimal truncation of a given size which
minimizes the error in the ground state energy. Ground state energies and
spin-spin correlations are obtained for clusters with up to thirty-two sites
without the need to restrict the symmetry of the structures. The results are
compared to full-space calculations and to unfrustrated structures based on the
honeycomb lattice.Comment: 22 pages and 12 Postscript figure
Report on the 2013 Rapid Assessment Survey of Marine Species at New England Bays and Harbors
Introduced species (i.e., non-native species that have become established in a new location) have increasingly been recognized as a concern as they have become more prevalent in marine and terrestrial environments (Mooney and Cleland 2001; Simberloff et al. 2005). The ability of introduced species to alter population, community, and ecosystem structure and function, as well as cause significant economic damage is well documented (Carlton 1989, 1996b, 2000; Cohen and Carlton 1995; Cohen et al. 1995; Elton 1958; Meinesz et al. 1993; Occhipinti-Ambrogi and Sheppard 2007; Pimentel et al. 2005; Thresher 2000). The annual economic costs incurred from managing the approximately 50,000 introduced species in the United States alone are estimated to be over $120 billion (Pimentel et al. 2005). Having a monitoring network in place to track new introductions and distributional changes of introduced species is critical for effective management, as these efforts may be more successful when species are detected before they have the chance to become established. A rapid assessment survey is one such method for early detection of introduced species. With rapid assessment surveys, a team of taxonomic experts record and monitor marine species–providing a baseline inventory of native, introduced, and cryptogenic (i.e., unknown origin) species (as defined by Carlton 1996a)–and document range expansions of previously identified species. Since 2000, five rapid assessment surveys have been conducted in New England. These surveys focus on recording species at marinas, which often are in close proximity to transportation vectors (i.e., recreational boats). Species are collected from floating docks and piers because these structures are accessible regardless of the tidal cycle. Another reason for sampling floating docks and other floating structures is that marine introduced species are often found to be more prevalent on artificial surfaces than natural surfaces (Glasby and Connell 2001; Paulay et al. 2002). The primary objectives of these surveys are to: (1) identify native, introduced, and cryptogenic marine species, (2) expand on data collected in past surveys, (3) assess the introduction status and range extensions of documented introduced species, and (4) detect new introductions. This report presents the introduced, cryptogenic, and native species recorded during the 2013 survey
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
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