148 research outputs found
Theory for the Ultrafast Structural Response of optically excited small clusters: Time-dependence of the Ionization Potential
Combining an electronic theory with molecular dynamics simulations we present
results for the ultrafast structural changes in small clusters. We determine
the time scale for the change from the linear to a triangular structure after
the photodetachment process Ag. We show that the
time-dependent change of the ionization potential reflects in detail the
internal degrees of freedom, in particular coherent and incoherent motion, and
that it is sensitive to the initial temperature. We compare with experiment and
point out the general significance of our results.Comment: 10 pages, Revtex, 3 postscript figure
Photoelectron spectra of aluminum cluster anions: Temperature effects and ab initio simulations
Photoelectron (PES) spectra from aluminum cluster anions (from 12 to 15
atoms) at various temperature regimes, were studied using ab-initio molecular
dynamics simulations and experimentally. The calculated PES spectra, obtained
via shifting of the simulated electronic densities of states by the
self-consistently determined values of the asymptotic exchange-correlation
potential, agree well with the measured ones, allowing reliable structural
assignments and theoretical estimation of the clusters' temperatures.Comment: RevTex, 3 gif figures. Scheduled for Oct 15, 1999, issue of Phys.
Rev. B as Rapid Communicatio
Structure and Magnetism of Neutral and Anionic Palladium Clusters
The properties of neutral and anionic Pd_N clusters were investigated with
spin-density-functional calculations. The ground state structures are
three-dimensional for N>3 and they are magnetic with a spin-triplet for 2<=N<=7
and a spin nonet for N=13 neutral clusters. Structural- and spin-isomers were
determined and an anomalous increase of the magnetic moment with temperature is
predicted for a Pd_7 ensemble. Vertical electron detachment and ionization
energies were calculated and the former agree well with measured values for
anionic Pd_N clusters.Comment: 5 pages, 3 figures, fig. 2 in color, accepted to Phys. Rev. Lett.
(2001
Optical response of small silver clusters
The time-dependent local density approximation is applied to the optical
response of the silver clusters, Ag_2, Ag_3, Ag_8 and Ag_9^+. The calculation
includes all the electrons beyond the closed-shell Ag^{+11} ionic core, thus
including for the first time explicitly the filled d-shell in the response. The
excitation energy of the strong surface plasmon near 4 eV agrees well with
experiment. The theoretical transition strength is quenched by a factor of 4
with respect to the pure s-electron sum rule in Ag_8 due to the d-electrons. A
comparable amount of strength lies in complex states below 6 eV excitation. The
total below 6 eV, about 50% of the s sum rule, is consistent with published
experiments.Comment: 13 pages RevTex and 9 Postscript figure
Ab initio studies of structures and properties of small potassium clusters
We have studied the structure and properties of potassium clusters containing
even number of atoms ranging from 2 to 20 at the ab initio level. The geometry
optimization calculations are performed using all-electron density functional
theory with gradient corrected exchange-correlation functional. Using these
optimized geometries we investigate the evolution of binding energy, ionization
potential, and static polarizability with the increasing size of the clusters.
The polarizabilities are calculated by employing Moller-Plesset perturbation
theory and time dependent density functional theory. The polarizabilities of
dimer and tetramer are also calculated by employing large basis set coupled
cluster theory with single and double excitations and perturbative triple
excitations. The time dependent density functional theory calculations of
polarizabilities are carried out with two different exchange-correlation
potentials: (i) an asymptotically correct model potential and (ii) within the
local density approximation. A systematic comparison with the other available
theoretical and experimental data for various properties of small potassium
clusters mentioned above has been performed. These comparisons reveal that both
the binding energy and the ionization potential obtained with gradient
corrected potential match quite well with the already published data.
Similarly, the polarizabilities obtained with Moller-Plesset perturbation
theory and with model potential are quite close to each other and also close to
experimental data.Comment: 33 pages including 10 figure
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