966 research outputs found
Photo-excitation of a light-harvesting supra-molecular triad: a Time-Dependent DFT study
We present the first time-dependent density-functional theory (TDDFT)
calculation on a light harvesting triad carotenoid-diaryl-porphyrin-C60.
Besides the numerical challenge that the ab initio study of the electronic
structure of such a large system presents, we show that TDDFT is able to
provide an accurate description of the excited state properties of the system.
In particular we calculate the photo-absorption spectrum of the supra-molecular
assembly, and we provide an interpretation of the photo-excitation mechanism in
terms of the properties of the component moieties. The spectrum is in good
agreement with experimental data, and provides useful insight on the
photo-induced charge transfer mechanism which characterizes the system.Comment: Accepted for publication on JPC, March 09th 200
Vibrational signatures for low-energy intermediate-sized Si clusters
We report low-energy locally stable structures for the clusters Si20 and Si21. The structures were obtained by performing geometry optimizations within the local density approximation. Our calculated binding energies for these clusters are larger than any previously reported for this size regime. To aid in the experimental identification of the structures, we have computed the full vibrational spectra of the clusters, along with the Raman and IR activities of the various modes using a recently developed first-principles technique. These represent, to our knowledge, the first calculations of Raman and IR spectra for Si clusters of this size
The Hamiltonian of the V Spin System from first-principles Density-Functional Calculations
We report first-principles all-electron density-functional based studies of
the electronic structure, magnetic ordering and anisotropy for the V
molecular magnet. From these calculations, we determine a Heisenberg
Hamiltonian with four antiferromagnetic and one {\em ferromagnetic} coupling.
We perform direct diagonalization to determine the temperature dependence of
the susceptibility. This Hamiltonian reproduces the experimentally observed
spin =1/2 ground state and low-lying =3/2 excited state. A small
anisotropy term is necessary to account for the temperature independent part of
the magnetization curve.Comment: 4 pages in RevTeX format + 2 ps-figures, accepted by PRL Feb. 2001
(previous version was an older version of the paper
The Puzzle of Sibling Attachment Non-Concordance: Implications of Categorical versus Continuous Approaches to Attachment
PURPOSE OF THE CURRENT STUDY: To determine whether characterizing the quality of attachment as a continuous measure impacts the extent to which siblings’ attachment relationships are judged concordant. To investigate whether continuous measures of attachment provide additional information regarding the similarity of more specific aspects of siblings attachment relationships
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
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
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
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
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
First-principles calculations of the self-trapped exciton in crystalline NaCl
The atomic and electronic structure of the lowest triplet state of the
off-center (C2v symmetry) self-trapped exciton (STE) in crystalline NaCl is
calculated using the local-spin-density (LSDA) approximation. In addition, the
Franck-Condon broadening of the luminescence peak and the a1g -> b3u absorption
peak are calculated and compared to experiment. LSDA accurately predicts
transition energies if the initial and final states are both localized or
delocalized, but 1 eV discrepancies with experiment occur if one state is
localized and the other is delocalized.Comment: 4 pages with 4 embeddded figure
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