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

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

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

EFFECTS OF ACIDITY AND METAL ENSEMBLE SIZE ON THE COKE FORMATION IN PT/NAY AND PTCU/NAY BY METHYLCYCLOPENTANE CONVERSION

Reduction of ion exchanged Pt2+ and Cu2+ ions with H2 forms metal atoms and protons of high Broensted acidity. The "coke" deposits formed during methylcyclopentane (MCP) conversion have been analyzed by temperature programmed oxidation (TPO). Acid sites are instrumental in ring enlargment of MCP; Cu atoms dilutePt ensembles required for ring opening. Coke deposits on metal and acid sites give rise to different TPO peaks, the high temperature peak increases with the concentration of Broensted sites. For high Cu/Pt ratios, coke formation on metal particles is negligible, showing that coke formation on metal surfaces is ensemble-specific