Two-step Liquid Drop Model for Binary, Metal-rich Clusters

It is shown that differences observed between the ionization potentials of the molecular-doped metallic clusters and those corresponding to the bare metallic ones can be explained by a two-step approach of the classical Liquid Drop Model. This approach takes into account the distinct physical properties of the interface between the molecular core and the metallic shell. Also, it is shown that the presence of the molecular core may act in the determination of the predominant channel of the coulombic fission.Comment: 8 page

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

Negative heat-capacity at phase-separations in microcanonical thermostatistics of macroscopic systems with either short or long-range interactions

Conventional thermo-statistics address infinite homogeneous systems within the canonical ensemble. However, some 170 years ago the original motivation of thermodynamics was the description of steam engines, i.e. boiling water. Its essential physics is the separation of the gas phase from the liquid. Of course, boiling water is inhomogeneous and as such cannot be treated by conventional thermo-statistics. Then it is not astonishing, that a phase transition of first order is signaled canonically by a Yang-Lee singularity. Thus it is only treated correctly by microcanonical Boltzmann-Planck statistics. This was elaborated in the talk presented at this conference. It turns out that the Boltzmann-Planck statistics is much richer and gives fundamental insight into statistical mechanics and especially into entropy. This can be done to a far extend rigorously and analytically. The deep and essential difference between ``extensive'' and ``intensive'' control parameters, i.e. microcanonical and canonical statistics, was exemplified by rotating, self-gravitating systems. In the present paper the necessary appearance of a convex entropy $S(E)$ and the negative heat capacity at phase separation in small as well macroscopic systems independently of the range of the force is pointed out.Comment: 6 pages, 1 figure, 1 table; contribution to the international conference "Next Sigma Phi" on news, expectations, and trends in statistical physics, Crete 200

Silver and oxygen: Transition from clusters to nanoparticles

AbstractBy varying the sizes of isolated and charged silver particles, we may observe a wide range of reactions from weak molecular-oxygen physisorption to strong oxygen chemisorption. The global electron configuration dominates the stability of the silver–oxygen complexes. Our experimental studies at 77 K show a cluster regime below 40 free valence electrons in the system. Here each atom of silver added to the complex cause strong alternations of the oxygen binding by quantum effects. Bigger silver–oxygen complexes show smoother size dependence. As is rather typical for nanoparticles, the quantum effects are here less important, while the system size still matters. The electrostatic interaction between the charge state of the nanoparticle and the charge transfer of the reaction accounts for the general trends observed at silver, as it is in related oxygen–metal complexes

Avant-propos

Le CNRS a été créé le 19 octobre 1939. La guerre en Europe venait d'éclater. Le gouvernement français souhaitait renforcer son potentiel scientifique. Depuis un demi-siècle, il cherchait la meilleure formule pour développer la recherche. Dans l'urgence, il appelait à l'effort national. Au lendemain de l'armistice de juin 1940, il fut question de supprimer un CNRS d'autant plus détesté qu'il semblait être la créature du Front populaire. Il survécut pourtant et connut, par la suite, bien des mé..

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

Semi-spheroidal Quantum Harmonic Oscillator

A new single-particle shell model is derived by solving the Schr\"odinger equation for a semi-spheroidal potential well. Only the negative parity states of the $Z(z)$ component of the wave function are allowed, so that new magic numbers are obtained for oblate semi-spheroids, semi-sphere and prolate semi-spheroids. The semi-spherical magic numbers are identical with those obtained at the oblate spheroidal superdeformed shape: 2, 6, 14, 26, 44, 68, 100, 140, ... The superdeformed prolate magic numbers of the semi-spheroidal shape are identical with those obtained at the spherical shape of the spheroidal harmonic oscillator: 2, 8, 20, 40, 70, 112, 168 ...Comment: 4 pages, 3 figures, 1 tabl

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