Semiclassical theory of surface plasmons in spheroidal clusters

A microscopic theory of linear response based on the Vlasov equation is extended to systems having spheroidal equilibrium shape. The solution of the linearized Vlasov equation, which gives a semiclassical version of the random phase approximation, is studied for electrons moving in a deformed equilibrium mean field. The deformed field has been approximated by a cavity of spheroidal shape, both prolate and oblate. Contrary to spherical systems, there is now a coupling among excitations of different multipolarity induced by the interaction among constituents. Explicit calculations are performed for the dipole response of deformed clusters of different size. In all cases studied here the photoabsorption strength for prolate clusters always displays a typical double-peaked structure. For oblate clusters we find that the high--frequency component of the plasmon doublet can get fragmented in the medium size region ($N \sim 250$). This fragmentation is related to the presence of two kinds of three-dimensional electron orbits in oblate cavities. The possible scaling of our semiclassical equations with the valence electron number and density is investigated.Comment: 23 pages, 8 figures, revised version, includes discussion of scalin

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 $\Delta$. We derive a simple analytic approximate expression determining $\Delta$ 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 $50 < N < 250$. A small surface roughness $\Delta\simeq 0.6$ \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.

Ionic and electronic structure of sodium clusters up to N=59

We determined the ionic and electronic structure of sodium clusters with even electron numbers and 2 to 59 atoms in axially averaged and three-dimensional density functional calculations. A local, phenomenological pseudopotential that reproduces important bulk and atomic properties and facilitates structure calculations has been developed. Photoabsorption spectra have been calculated for $\mathrm{Na}_2$, $\mathrm{Na}_8$, and $\mathrm{Na}_9^+$ to $\mathrm{Na}_{59}^+$. The consistent inclusion of ionic structure considerably improves agreement with experiment. An icosahedral growth pattern is observed for $\mathrm{Na}_{19}^+$ to $\mathrm{Na}_{59}^+$. This finding is supported by photoabsorption data.Comment: To appear in Phys. Rev. B 62. Version with figures in better quality can be requested from the author

Unified description of magic numbers of metal clusters in terms of the 3-dimensional q-deformed harmonic oscillator

Magic numbers predicted by a 3-dimensional q-deformed harmonic oscillator with Uq(3)>SOq(3) symmetry are compared to experimental data for atomic clusters of alkali metals (Li, Na, K, Rb, Cs), noble metals (Cu, Ag, Au), divalent metals (Zn, Cd), and trivalent metals (Al, In), as well as to theoretical predictions of jellium models, Woods-Saxon and wine bottle potentials, and to the classification scheme using the 3n+l pseudo quantum number. In alkali metal clusters and noble metal clusters the 3-dimensional q-deformed harmonic oscillator correctly predicts all experimentally observed magic numbers up to 1500 (which is the expected limit of validity for theories based on the filling of electronic shells), while in addition it gives satisfactory results for the magic numbers of clusters of divalent metals and trivalent metals, thus indicating that Uq(3), which is a nonlinear extension of the U(3) symmetry of the spherical (3-dimensional isotropic) harmonic oscillator, is a good candidate for being the symmetry of systems of several metal clusters. The Taylor expansions of angular momentum dependent potentials approximately producing the same spectrum as the 3-dimensional q-deformed harmonic oscillator are found to be similar to the Taylor expansions of the symmetrized Woods-Saxon and wine-bottle symmetrized Woods-Saxon potentials, which are known to provide successful fits of the Ekardt potentials.Comment: 23 pages including 7 table