182 research outputs found
Charge-Induced Fragmentation of Sodium Clusters
The fission of highly charged sodium clusters with fissilities X>1 is studied
by {\em ab initio} molecular dynamics. Na_{24}^{4+} is found to undergo
predominantly sequential Na_{3}^{+} emission on a time scale of 1 ps, while
Na_{24}^{Q+} (5 \leq Q \leq 8) undergoes multifragmentation on a time scale
\geq 0.1 ps, with Na^{+} increasingly the dominant fragment as Q increases. All
singly-charged fragments Na_{n}^{+} up to size n=6 are observed. The observed
fragment spectrum is, within statistical error, independent of the temperature
T of the parent cluster for T \leq 1500 K. These findings are consistent with
and explain recent trends observed experimentally.Comment: To appear in Physical Review Letter
Size effect in the ionization energy of PAH clusters
We report the first experimental measurement of the near-threshold
photo-ionization spectra of polycyclic aromatic hydrocarbon clusters made of
pyrene C16H10 and coronene C24H12, obtained using imaging photoelectron
photoion coincidence spectrometry with a VUV synchrotron beamline. The
experimental results of the ionization energy are confronted to calculated ones
obtained from simulations using dedicated electronic structure treatment for
large ionized molecular clusters. Experiment and theory consistently find a
decrease of the ionization energy with cluster size. The inclusion of
temperature effects in the simulations leads to a lowering of this energy and
to a quantitative agreement with the experiment. In the case of pyrene, both
theory and experiment show a discontinuity in the IE trend for the hexamer
Electronic entropy, shell structure, and size-evolutionary patterns of metal clusters
We show that electronic-entropy effects in the size-evolutionary patterns of
relatively small (as small as 20 atoms), simple-metal clusters become prominent
already at moderate temperatures. Detailed agreement between our
finite-temperature-shell-correction-method calculations and experimental
results is obtained for certain temperatures. This agreement includes a
size-dependent smearing out of fine-structure features, accompanied by a
measurable reduction of the heights of the steps marking major-shell and
subshell closings, thus allowing for a quantitative analysis of cluster
temperatures.Comment: Latex/Revtex, 4 pages with 3 Postscript figure
Structure and properties of small sodium clusters
We have investigated structure and properties of small metal clusters using
all-electron ab initio theoretical methods based on the Hartree-Fock
approximation and density functional theory, perturbation theory and compared
results of our calculations with the available experimental data and the
results of other theoretical works. We have systematically calculated the
optimized geometries of neutral and singly charged sodium clusters having up to
20 atoms, their multipole moments (dipole and quadrupole), static
polarizabilities, binding energies per atom, ionization potentials and
frequencies of normal vibration modes. Our calculations demonstrate the great
role of many-electron correlations in the formation of electronic and ionic
structure of small metal clusters and form a good basis for further detailed
study of their dynamic properties, as well as structure and properties of other
atomic cluster systems.Comment: 47 pages, 16 figure
Rearrangement of cluster structure during fission processes
Results of molecular dynamics simulations of fission reactions and are presented. Dependence
of the fission barriers on isomer structure of the parent cluster is analyzed.
It is demonstrated that the energy necessary for removing homothetic groups of
atoms from the parent cluster is largely independent of the isomer form of the
parent cluster. Importance of rearrangement of the cluster structure during the
fission process is elucidated. This rearrangement may include transition to
another isomer state of the parent cluster before actual separation of the
daughter fragments begins and/or forming a "neck" between the separating
fragments
Molecular dynamics in shape space and femtosecond vibrational spectroscopy of metal clusters
We introduce a method of molecular dynamics in shape space aimed at metal
clusters. The ionic degrees of freedom are described via a dynamically
deformable jellium with inertia parameters derived from an incompressible,
irrotational flow. The shell correction method is used to calculate the
electronic potential energy surface underlying the dynamics. Our finite
temperature simulations of Ag_14 and its ions, following the negative to
neutral to positive scheme, demonstrate the potential of pump and probe
ultrashort laser pulses as a spectroscopy of cluster shape vibrations.Comment: Latex/Revtex, 4 pages with 3 Postscript figure
Curvature effect on the interaction between folded graphitic surface and silver clusters
Evidence of curvature effects on the interaction and binding of silver
clusters on folded graphitic surfaces has been shown from both experiment and
theory. Density Functional Theory (DFT) calculations within the local density
and generalized gradient approximations have been performed for the structural
relaxation of both Ag and Ag on curved surfaces, showing a cross-over from
quantum to classical behaviour. Using Lennard-Jones potential to model the
interaction between a single cluster and the graphene surface, evidence is
found for the curvature effect on the binding of silver nano-particles to
folding graphitic surfaces. The theoretical results are compared to SEM and AFM
images of samples obtained from pre-formed silver cluster deposition on
carboneous substrates exhibiting anisotropic pleat structures
Rough droplet model for spherical metal clusters
We study the thermally activated oscillations, or capillary waves, of a
neutral metal cluster within the liquid drop model. These deformations
correspond to a surface roughness which we characterize by a single parameter
. We derive a simple analytic approximate expression determining
as a function of temperature and cluster size. We then estimate the
induced effects on shell structure by means of a periodic orbit analysis and
compare with recent data for shell energy of sodium clusters in the size range
. A small surface roughness \AA~ is seen to
give a reasonable account of the decrease of amplitude of the shell structure
observed in experiment. Moreover -- contrary to usual Jahn-Teller type of
deformations -- roughness correctly reproduces the shape of the shell energy in
the domain of sizes considered in experiment.Comment: 20 pages, 4 figures, important modifications of the presentation, to
appear in Phys. Rev.
Photoionization profiles of metal clusters and the Fowler formula
Metal cluster ionization potentials are important characteristics of these
"artificial atoms," but extracting these quantities from cluster
photoabsorption spectra, especially in the presence of thermal smearing,
remains a big challenge. Here we demonstrate that the classic Fowler theory of
surface photoemission does an excellent job of fitting the photoabsorption
profile shapes of neutral In_{n=3-34} clusters [Wucher et al., New J. Phys. 10,
103007 (2008)]. The deduced ionization potentials extrapolate precisely to the
bulk work function, and the internal cluster temperatures are in close
agreement with values expected for an ensemble of freely evaporating clusters.
Supplementing an earlier application to potassium clusters, these results
suggest that the Fowler formalism, which is straightforward and physical, may
be of significant utility in metal cluster spectroscopy. It is hoped also that
the results will encourage a comprehensive theoretical analysis of the
applicability of bulk-derived models to cluster photoionization behavior, and
of the transition from atomic and molecular-type to surface-type photoemission
Supershells in Metal Clusters: Self-Consistent Calculations and their Semiclassical Interpretation
To understand the electronic shell- and supershell-structure in large metal
clusters we have performed self-consistent calculations in the homogeneous,
spherical jellium model for a variety of different materials. A scaling
analysis of the results reveals a surprisingly simple dependence of the
supershells on the jellium density. It is shown how this can be understood in
the framework of a periodic-orbit-expansion by analytically extending the
well-known semiclassical treatment of a spherical cavity to more realistic
potentials.Comment: 4 pages, revtex, 3 eps figures included, for additional information
see http://radix2.mpi-stuttgart.mpg.de/koch/Diss
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