1,053 research outputs found
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
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
Direct Minimization Generating Electronic States with Proper Occupation Numbers
We carry out the direct minimization of the energy functional proposed by
Mauri, Galli and Car to derive the correct self-consistent ground state with
fractional occupation numbers for a system degenerating at the Fermi level. As
a consequence, this approach enables us to determine the electronic structure
of metallic systems to a high degree of accuracy without the aid of level
broadening of the Fermi-distribution function. The efficiency of the method is
illustrated by calculating the ground-state energy of C and Si
molecules and the W(110) surface to which a tungsten adatom is adsorbed.Comment: 4 pages, 4 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
Quasi one dimensional He inside carbon nanotubes
We report results of diffusion Monte Carlo calculations for both He
absorbed in a narrow single walled carbon nanotube (R = 3.42 \AA) and strictly
one dimensional He. Inside the tube, the binding energy of liquid He is
approximately three times larger than on planar graphite. At low linear
densities, He in a nanotube is an experimental realization of a
one-dimensional quantum fluid. However, when the density increases the
structural and energetic properties of both systems differ. At high density, a
quasi-continuous liquid-solid phase transition is observed in both cases.Comment: 11 pages, 3ps figures, to appear in Phys. Rev. B (RC
Size Effects in Carbon Nanotubes
The inter-shell spacing of multi-walled carbon nanotubes was determined by
analyzing the high resolution transmission electron microscopy images of these
nanotubes. For the nanotubes that were studied, the inter-shell spacing
is found to range from 0.34 to 0.39 nm, increasing with
decreasing tube diameter. A model based on the results from real space image
analysis is used to explain the variation in inter-shell spacings obtained from
reciprocal space periodicity analysis. The increase in inter-shell spacing with
decreased nanotube diameter is attributed to the high curvature, resulting in
an increased repulsive force, associated with the decreased diameter of the
nanotube shells.Comment: 4 pages. RevTeX. 4 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
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
Semiconductive and Photoconductive Properties of the Single Molecule Magnets Mn-Acetate and FeBr
Resistivity measurements are reported for single crystals of
Mn-Acetate and FeBr. Both materials exhibit a
semiconductor-like, thermally activated behavior over the 200-300 K range. The
activation energy, , obtained for Mn-Acetate was 0.37 0.05
eV, which is to be contrasted with the value of 0.55 eV deduced from the
earlier reported absorption edge measurements and the range of 0.3-1 eV from
intramolecular density of states calculations, assuming = , the
optical band gap. For FeBr, was measured as 0.73 0.1 eV,
and is discussed in light of the available approximate band structure
calculations. Some plausible pathways are indicated based on the crystal
structures of both lattices. For Mn-Acetate, we also measured
photoconductivity in the visible range; the conductivity increased by a factor
of about eight on increasing the photon energy from 632.8 nm (red) to 488 nm
(blue). X-ray irradiation increased the resistivity, but was insensitive
to exposure.Comment: 7 pages, 8 figure
Maximally-localized generalized Wannier functions for composite energy bands
We discuss a method for determining the optimally-localized set of
generalized Wannier functions associated with a set of Bloch bands in a
crystalline solid. By ``generalized Wannier functions'' we mean a set of
localized orthonormal orbitals spanning the same space as the specified set of
Bloch bands. Although we minimize a functional that represents the total spread
sum_n [ _n - _n^2 ] of the Wannier functions in real space, our method
proceeds directly from the Bloch functions as represented on a mesh of
k-points, and carries out the minimization in a space of unitary matrices
U_mn^k describing the rotation among the Bloch bands at each k-point. The
method is thus suitable for use in connection with conventional
electronic-structure codes. The procedure also returns the total electric
polarization as well as the location of each Wannier center. Sample results for
Si, GaAs, molecular C2H4, and LiCl will be presented.Comment: 22 pages, two-column style with 4 postscript figures embedded. Uses
REVTEX and epsf macros. Also available at
http://www.physics.rutgers.edu/~dhv/preprints/index.html#nm_wan
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