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  • 36.40  (55)
  • Springer  (55)
  • American Association for the Advancement of Science
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  • 1990-1994  (55)
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  • 1925-1929
  • 1993  (55)
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  • Springer  (55)
  • American Association for the Advancement of Science
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  • 2010-2014
  • 2005-2009
  • 1990-1994  (55)
  • 1980-1984
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  • 1
    ISSN: 1432-0630
    Keywords: 36.40 ; 61.1.P ; 68.20
    Source: Springer Online Journal Archives 1860-2000
    Topics: Mechanical Engineering, Materials Science, Production Engineering, Mining and Metallurgy, Traffic Engineering, Precision Mechanics , Physics
    Notes: Abstract Fullerene powder mixtures with different C60/C70 ratios have been analyzed by a variety of techniques, and results have been compared. The fullerence mixtures have been characterized as solutions in n-hexane by high-pressure liquid chromatography (HPLC) and UV-VIS spectroscopy. Thin films of fullerenes on Au(111) have been prepared from the mixtures by sublimation. The sublimation process has been studied by simultaneous thermogravimetric and differential thermal analyses. Thin fullerene films on Au(111) have been investigated by scanning tunneling microscopy (STM). The STM images show primarily two types of ballshaped molecules arranged in a lattice with hexagonal symmetry (fcc(111) face, nearest neighbour distance: 1 nm). The two species differ in diameter. STM images of films made of mixtures of different C60/C70 ratios show that C70 molecules display a larger apparent diameter (0.8 nm) and corrugation than C60 molecules (0.7 nm). The C60/C70 ratios obtained by counting the corresponding molecular species in the STM images of the thin films are compared to the C60/C70 ratios determined by HPLC on hexane solutions of the mixtures. The observed differences might be explained by different rates of sublimation for the two species. The STM images reveal film defects (vacancies and boundaries) and dynamic processes (displacement of C70 molecules and vacancies). In films prepared to have a C60 coverage of less than one monolayer, stable structural units of the C60(111) surface consisting of three or seven C60 molecules are revealed by STM. Occasionally, substructure within individual fullerene molecules is observed.
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  • 2
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    The European physical journal 26 (1993), S. 175-177 
    ISSN: 1434-6079
    Keywords: 36.40 ; 67.90+Z ; 71.90+Q
    Source: Springer Online Journal Archives 1860-2000
    Topics: Physics
    Notes: Abstract Excitation and decay processes of helium clusters are investigated with fluorescence methods. The results differ remarkably from that obtained for the heavier rare gas clusters. They are discussed in view of the unusual structural and electronic properties of helium.
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  • 3
    ISSN: 1434-6079
    Keywords: 76.60 ; 03.65.F ; 36.40
    Source: Springer Online Journal Archives 1860-2000
    Topics: Physics
    Notes: Abstract For both highern andI i ≧1 spin clusters, combinatorics provides powerful arguments with which to investigate the substructural forms of cluster spin algebras; this is especially so for SO(3) ×l n symmetries for 12≦n≦60 wherex (.) [λ] character tabulations become extensive. Bijective enumerative mappings over the combinatorialp-tuples (number partitions) afford insight into the general functionf(p,n) as well as into {|IM(I 1−I n [λ]〉} M -structure of spin algebras, even where the full details of the explicitx () [λ] (l n ) characters are not readily available. Both simply-reducible and higher aspects ofl n -inner tensor product (ITP) algebras are derived from dimensionality considerations, as part of combinatorial hooklength formalisms for $$\chi _{(1^n )}^{[\lambda ]} $$ . TheI i ≦3/2 forms of [A] n clusters forn≦20, (forp≦3, 4) of multiple-quantum NMR (MQ-NMR) are considered here as part of current interest in giant cage-clusters. In addition, the SU2 substructural hierarchy over Liouville space is derived for [A]20(l n ) (I i =1/2) spin cluster of the cage-cluster molecule dodecahedrane; aspects ofI i =1 spin cluster over {|IM (...)〉} space are derived as high temperature model of the exo-cage of [H2O]+ @[H2O]20 cluster ion; 20-fold higher-I i lusters provide models for M @M20 metal-clusters and further applications ofl 20-number partitions.
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  • 4
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    The European physical journal 26 (1993), S. 255-257 
    ISSN: 1434-6079
    Keywords: 36.40
    Source: Springer Online Journal Archives 1860-2000
    Topics: Physics
    Notes: Abstract Molecular dynamics is used to study the melting and structural transitions of small copper clusters. The melting temperature is found to be proportional to the average coordination number. Small icosahedral clusters melt at slightly higher temperatures than the cubic structures. Small cuboctahedral clusters are not stable but transform via a nondiffusive transition to icosahedral structure.
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  • 5
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    The European physical journal 26 (1993), S. 261-263 
    ISSN: 1434-6079
    Keywords: 36.40
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    Topics: Physics
    Notes: Abstract We apply the nuclear shell model to jellium clusters of up to twenty-one Na atoms. Binding energies, ionization potentials, and photoabsorption cross sections are calculated and compared with mean-field results.
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  • 6
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    The European physical journal 26 (1993), S. 322-324 
    ISSN: 1434-6079
    Keywords: 36.40 ; 33.80.E
    Source: Springer Online Journal Archives 1860-2000
    Topics: Physics
    Notes: Abstract The ionization potentials of AlnCom clusters (n〉m) have been bracketed using laser photoionization mass spectrometry. We find the electronic shell structure manifested in the ionization potentials of Aln for n≥7 is observed also for AlnCo and AlnCo2, and is consistent with cobalt contributing one electron to the conduction band of the cluster. However, with increasing number of cobalt atoms, this simple picture breaks down; all vestiges of aluminum cluster electronic shell structure are absent for m≥4.
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  • 7
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    The European physical journal 26 (1993), S. 364-366 
    ISSN: 1434-6079
    Keywords: 36.40 ; 64.60.Qb ; 64.70.Kb ; 82.20.Wt
    Source: Springer Online Journal Archives 1860-2000
    Topics: Physics
    Notes: Abstract Simulations of clusters containing 100 to 250 molecules of TeF6 successfully reproduce the crystalline packing arrangements observed in electron diffraction investigations of large molecular clusters (∼ 104 molecules) of the same material. More remarkably, when the clusters are cooled step by step in MD computations at a rate of ca. 1011 K/s they spontaneously undergo the same bcc to monoclinic phase transition that has been observed experimentally in supersonic flow, despite the million-fold difference in the timescales involved. The existence of such a correspondence over so many orders of magnitude, in itself, imposes severe constraints on what type of molecular mechanism can underlie the transformation. Even more revealing evidence about the molecular behavior associated with the phase change is provided by the simulations. They show the formation of the actual transition complexes along the transition pathway, namely, the critical nuclei of the new phase. These nuclei, which are made up of approximately 20 molecules, can be recognized in the midst of the surrounding matter. Techniques based on molecular orientations, involving Pawley-Fuchs projections and orientational angular distribution functions, make it possible to estimate the size of critical nuclei. One noteworthy result established in the simulations is that the solid-state transition temperature from bcc to monoclinic depends upon particle size in the same manner as does the freezing point.
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  • 8
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    The European physical journal 26 (1993), S. 382-384 
    ISSN: 1434-6079
    Keywords: 36.40 ; 67.90+Z ; 71.90+Q
    Source: Springer Online Journal Archives 1860-2000
    Topics: Physics
    Notes: Abstract Excitation and decay processes of helium clusters are investigated with fluorescence methods. The results differ remarkably from that obtained for the heavier rare gas clusters. They are discussed in view of the unusual structural and electronic properties of helium.
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  • 9
    ISSN: 1434-6079
    Keywords: 79.20N ; 36.40
    Source: Springer Online Journal Archives 1860-2000
    Topics: Physics
    Notes: Abstract The emission of neutral and positively charged silver clusters during sputtering of a polycrystalline silver target by 5 keV Ar+ ion bombardment has been studied and the sputter ejected silver flux has been characterized. As a result, the silver flux is found to be strongly dominated byneutral clusters rather than cluster ions. The contribution of neutral clusters in the overall silver flux decreases rapidly and monotonically with increasing cluster size n and decreases, in addition, with decreasing bombarding energy. The well known alternation of the secondary ion intensities of Ag n + as a function of cluster size (higher intensities for odd n) is found to be correlated with the effective “ionization potentials” of the corresponding sputtered neutral clusters.
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  • 10
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    The European physical journal 26 (1993), S. 134-136 
    ISSN: 1434-6079
    Keywords: 36.40
    Source: Springer Online Journal Archives 1860-2000
    Topics: Physics
    Notes: Abstract The melting properties of Ben, n=7−14, clusters have been studied using molecular dynamics simulations and an interatomic potential which contains two- and three-body terms, derived from local spin density calculations. The cluster meltinglike behavior has been studied calculating characteristic physical quantities like short-time averages of the kinetic energy per particle as a function of time, caloric curves and root-mean-square bond length fluctuations as a function of the cluster total energy. The meltinglike transition in Ben clusters shows more complex features than those found in van der Waals and ionic clusters. The estimated melting temperatures for n=11−14 are higher than the bulk value. This result indicates that the parameters of the cluster interaction potential could be inadequate to describe the thermodynamic properties of Ben clusters.
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  • 11
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    The European physical journal 26 (1993), S. 162-164 
    ISSN: 1434-6079
    Keywords: 36.40
    Source: Springer Online Journal Archives 1860-2000
    Topics: Physics
    Notes: Abstract The interaction of matrix-isolated silver clusters with CO has been investigated for clusters containing as few as 100 atoms/cluster. A vibrational mode at a monolayer coverage, which is found on bulk silver at 2110 cm−1, is present even for these small particles. For these small-sized particles however, an additional, broad, unresolved band at 1950 cm−1 appears, which does not exist for larger clusters. Whether this band has its origin in a modified chemical behaviour for particles smaller than 100 at/cl is not clear.
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  • 12
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    The European physical journal 26 (1993), S. 246-248 
    ISSN: 1434-6079
    Keywords: 82.30.N ; 36.40 ; 82.50.F
    Source: Springer Online Journal Archives 1860-2000
    Topics: Physics
    Notes: Abstract Tantalum sulfide cluster ions were produced by direct laser ablation, and were studied with a tandem time-of-flight mass spectrometer. The main dissociation channel of the UV-photolysis (248 nm) of tantalum sulfide cluster ions is sequent S2 loss. Structures with Ta3S4 and Ta4S6 as frameworks were suggested for the large tantalum sulfide cluster ions.
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  • 13
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    The European physical journal 26 (1993), S. 258-260 
    ISSN: 1434-6079
    Keywords: 36.40
    Source: Springer Online Journal Archives 1860-2000
    Topics: Physics
    Notes: Abstract A hypothetical ring-stacking procedure combined with the isolated-pentagon rule(IPR) shows variety of formation pathways of many fullerene structures with a 5- and 6-membered ring carbon cage. Combining the ring-stacking procedure with energetic considerations, the numbers of possible reaction channels are dramatically reduced within the framework of the ring-stacking considerations. This, in turn, gives the results that only some specific isomers of large fullerenes are selectively produced. The resulting fullerene structures specified are surprisingly well consistent with the recent experimental results.
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  • 14
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    The European physical journal 26 (1993), S. 12-14 
    ISSN: 1434-6079
    Keywords: 36.40
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    Topics: Physics
    Notes: Abstract We investigate the electronic and structural properties of small (N ≲ 20) and medium sized (N ≲ 500) clusters of Cu, using the first principles Tight-Binding Linear Muffin-Tin Orbitals (TB-LMTO) method in connection with the real-space recursion scheme. We find the electronic structure resembling the one of simple alkali metal clusters: Pronounced shell closing effects can be identified in the ionization potentials as well as in the HOMO-LUMO gaps for the magic sizesN=8, 20, 34 and 40. The low-energy equilibrium geometries show considerable Jahn-Teller distortions, just as in the case of alkali metals.
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  • 15
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    The European physical journal 26 (1993), S. 294-296 
    ISSN: 1434-6079
    Keywords: 36.40 ; 34.80
    Source: Springer Online Journal Archives 1860-2000
    Topics: Physics
    Notes: Abstract Electron energy loss spectroscopy has been performed with samples of pure C60 and C70 using primary electron energies between 10 and 1100 eV. The experimental data could be explained in terms of optically forbidden and allowed transitions, and by collective excitations (plasmons), which could be distinguished by their dependence on the energy of the primary electron.
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  • 16
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    The European physical journal 26 (1993), S. 305-307 
    ISSN: 1434-6079
    Keywords: 36.40 ; 35.20
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    Topics: Physics
    Notes: Abstract Carbon cluster ions generated by laser evaporation have been reacted with atoms (Ar) and molecules (O2, D2). In order to vary the reaction conditions for the cluster ions two gas inlets at different locations have been added to the cluster source. Addition of D2 increased the line width in the TOF-spectrum indicating the appearance of reaction products of the type CmDn. Both O2 and D2 proved very effective in removing the odd numbered carbon cluster ions in the vicinity of C60. Application of O2 produced a significant effect: depending on the gas pressure it reacted with small cluster ions forming products like CnO+ and CnO2 +. Such reaction channels are not found for n〉12 thus indicating a change in cluster geometry. Another sequence of experiments has been undertaken by adding Ar atoms to the carbon cluster ions. Some stable ionic reaction products like ArC+,..., ArC4 +, ArC5 + can be detected. It is known from previous studies that the ArC+ is a stable ion with an dissociation energy of about 1 eV.
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  • 17
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    The European physical journal 26 (1993), S. 320-322 
    ISSN: 1434-6079
    Keywords: 36.40
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    Topics: Physics
    Notes: Abstract Collision induced electron detachment of the fullerene C 60 − and the other C 60 − produced through the laser vaporization of a carbon rod was studied. Both of C 60 − showed quite different behavior for the process. It was suggested that the laser vaporized C 60 − has a different structure from the fullerence C 60 − .
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  • 18
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    The European physical journal 26 (1993), S. 329-331 
    ISSN: 1434-6079
    Keywords: 36.40 ; 31.20.D
    Source: Springer Online Journal Archives 1860-2000
    Topics: Physics
    Notes: Abstract The structures and stabilities of small mixed clusters of ammonia with hydrogen cyanide have been studied usingab initio electronic structure calculations at the Hartree Fock and Møller Plesset levels of theory. Stable structures for (NH3)nHCN, n=1, 2, 3 have been located. Two stable structures and a transition state for the heterodimer are described.
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  • 19
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    The European physical journal 26 (1993), S. 69-73 
    ISSN: 1434-6079
    Keywords: 36.40
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    Topics: Physics
    Notes: Abstract A novel picture of growth of fullerene and fullerene-like structures is proposed. The ring stacking model have been studied in detail in connection with the stability, structures and growth mechanism of carbon 5-and 6-membered ring network. Combining the model with energetic considerations, the selective formation of sizes and isomers of large fullerenes has successfully been described.
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  • 20
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    The European physical journal 26 (1993), S. 1-7 
    ISSN: 1434-6079
    Keywords: 36.40
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    Topics: Physics
    Notes: Abstract Two different approaches for studying the electronic structure of clusters are presented. The physical probe uses the photoexcitation of size selected alkali-atom clusters. Giant resonances govern the absorption cross-section. It is due to the collective excitation of delocalized valence electrons. The behavior of the resonance up to large sizes, 900-atom clusters for potassium and 1500-atom clusters for lithium puts into evidence the failure of the jellium model for lithium. The chemical approach makes use of the nucleation process in the presence of oxygen. From the analysis of mass spectra of oxidized products, informations are gained on the valence of metallic atom in the cluster oxide. The method is applied to europium and thulium clusters. A comparison is done with the simple case of alkali clusters.
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  • 21
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    The European physical journal 26 (1993), S. 370-372 
    ISSN: 1434-6079
    Keywords: 36.40 ; 78.55-M
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    Topics: Physics
    Notes: Abstract Excitation and decay processes of neutral and ionized ArN clusters are analysed using fluorescence spectroscopy with synchrotron radiation. The fluorescence yield of ionized ArN clusters is resonantly enhanced after excitation from states related to the atomic 3s levels.
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  • 22
    ISSN: 1434-6079
    Keywords: 36.40
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    Topics: Physics
    Notes: Abstract An apparatus for getting size selected and focused neutral carbon clusters was developed. Using image intensified charge coupled device (ICCD) system, the beam profiles of C 10 − and C10 were investigated. The results indicated that the beam density of C10 surpasses that of C 10 − of space charge limit.
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  • 23
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    The European physical journal 26 (1993), S. 323-325 
    ISSN: 1434-6079
    Keywords: 33.10.C ; 36.40 ; 77.40 ; 78.40.D
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    Topics: Physics
    Notes: Abstract Just what can be learned about cluster dynamics (and, more generally, about solvation dynamics) from spectral studies of small clusters that have been doped with a chromophore is still an open question. In the present work we suggest a novel procedure for calculating the shift in the electronic absorption spectrum of a chromophore deriving from the attachment to or the incorporation in a cluster. The particular system of interest here is benzene·Ar n , for which experimental results are readily available although their interpretation has been a point of controversy. In addition, since the present formalism is equally applicable to a chromophore isolated in a bulk phase (either liquid or solid), we are able to venture an explanation for the apparent observation that the spectral shift of cluster-isolated benzene does not approach the asymptotic values characteristic of the bulk-isolated species.
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  • 24
    ISSN: 1434-6079
    Keywords: 31.20.D ; 36.40 ; 82.40.W
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    Topics: Physics
    Notes: Abstract Electronic structure calculations employingab initio methods have been carried out for the H2S monomer and two of its associated dimers: its homodimer, (H2S)2 and its heterodimer with water. The results reported here include geometric parameters, the zero-point and minimum energies, rotational and vibrational constants, and dipole moments. The contribution of the monomers to the dimer spectrum has been suggested. Two structures for the homodimer corresponding to potential surface stationary points have been found. One of these has been identified as a transition state.
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  • 25
    ISSN: 1434-6079
    Keywords: 36.40
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    Topics: Physics
    Notes: Abstract Recently we demonstrated the formation of crystalline nanometer scale GaAs clusters from organometallic precursors using an aerosol process derived from organometallic vapor phase epitaxy (OMVPE) [P. C. Sercelet al., Appl Phys. Lett.61, 696 (1992)]. Here, we explore the influence of precracking the Ga precursor (trimethyl-gallium), forming nanometer scale Ga droplets, prior to introduction of AsH3 to the reaction. We find the GaAs clusters so formed have an entirely different morphology than do those formed when the reactants are pre-mixed prior to reaction. This data supports our earlier contention that homogeneous nucleation is the dominant reaction mechanism for the formation of the clusters.
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  • 26
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    The European physical journal 26 (1993), S. 1-3 
    ISSN: 1434-6079
    Keywords: 36.40 ; 33.20K
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    Topics: Physics
    Notes: Abstract We present optical extinction spectra of ligand-stabilized Au-clusters AuN with sizes of N=13 and N=55. They are compared to larger, embedded clusters up to N=5·103 (diameter 5nm). The Mie resonance due to excitation of the dipole plasmon polariton vanishes with decreasing cluster size. For N〉55, this effect has recently been interpreted as caused by smearing out of the interband transition edge of Au.
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  • 27
    ISSN: 1434-6079
    Keywords: 36.40 ; 31.20.Gm ; 31.20.D ; 82.40.We
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    Topics: Physics
    Notes: Abstract The structure and stability of the mixed clusters SO2(H2O)n, n ranging from 1 to 4, have been examined using semi-empirical quantum mechanical Hartree Fock methods with the improved PM3 parameter set as implemented in MOPAC [1]. Limited molecular dynamics studies together with investigation of the potential surface reveal potential barriers of 1 kcal/mol or less between many of the stable structures for a cluster of a given size. For n=1,2 the results are compared with those ofab initio calculations using a double zeta basis at the MP4 level.
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  • 28
    ISSN: 1434-6079
    Keywords: 36.40 ; 34.70.+e
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    Topics: Physics
    Notes: Abstract We have studied electron transfer from state-selected Rydberg atoms to (CS2) N and CS2(Ar) N clusters and compared the results to Rydberg electron transfer to isolated CS2 molecules. At large Rydberg principal quantum numbers (n〉20), the influence of the positive ionic core becomes negligible and we are able to directly investigate the competition between electronic autodetachment of the anions and intracluster energy exchanges between the anions and their environment. We show that argon atoms are unable to achieve efficient internal energy exchanges in heterogeneous clusters as compared to the high efficiency of CS2 molecules in homogeneous clusters.
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  • 29
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    The European physical journal 28 (1993), S. 73-80 
    ISSN: 1434-6079
    Keywords: 36.40 ; 71.70.G
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    Topics: Physics
    Notes: Abstract Hartree-Fock calculations are done for finite number of valence electrons (8, 20, 40, and 58) in a positively charged uniform background (jellium) with the density of bulk sodium. Differences and similarities with the results of Kohn-Sham local-density calculations are discussed. State-dependence and suppression of the wave functions are the two important effects coming from the nonlocality of the Hartree-Fock potential. These two effects, however, cancel in the density profile of electrons. The Kohn-Sham calculations consequently produce similar density profiles as in the Hartree-Fock calculations. The dipole polarizability is also calculated for 8-mers. The calculated value is still smaller than the measured one and is not an improvement of the insufficient Kohn-Sham result.
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  • 30
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    The European physical journal 26 (1993), S. 232-235 
    ISSN: 1434-6079
    Keywords: 31.20.D ; 31.30 ; 36.40
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    Topics: Physics
    Notes: Abstract This paper reports results obtained in the study of small alkali metal clusters (2≤n≤34). Properties of interest include static descriptions of the Potential Energy Surfaces (PES) using a Distance-Dependent Tight Binding hamiltonian (DDTB) and new results obtained with the same hamiltonian through a Monte-Carlo Growth Method (MCGM) which is shown to give an efficient way to sample the PES, but may also be helpful to estimate the statistical occurrences of the various isomers (catching areas). The probability for generating a given configuration is proportional to a Boltzmann distribution factor and hence a temperature dependence is introduced in the study of the PES. In section 2, the temperature dependence of the optical response for small clusters (on the example of Na4) is simulated throughab initio calculations of the electronic structure coupled with Monte-Carlo dynamics on the absorbing system in the ground state.
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  • 31
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    The European physical journal 26 (1993), S. 220-222 
    ISSN: 1434-6079
    Keywords: 36.40 ; 33.80 ; 35.20
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    Topics: Physics
    Notes: Abstract Picosecond multiphoton ionization of (NO)mArn clusters produced in a supersonic expansion of NO/Ar gas mixtures has been studied using time-of-flight mass spectrometry. Two-photon ionization with 266 nm photons show that dilute gas mixtures (1% NO/Ar) yield clusters limited to m≤7, but with as many as 37 argon atoms. Magic numbers are observed for NO+Ar12, NO+Ar18, (NO) 2 + Ar17, NO+Ar22, and (NO) 2 + Ar21 and are understood in terms of solvation of the NO+ and (NO) 2 + by argon in icosahedral arrangements. Four-photon ionization with 532 nm light produces dissociation of the clusters to yield only NO+Arn with n up to 54. This distribution exhibits an additional magic number at n=54, consistent with the completion of a second solvation sphere about the NO+. The known wavelength dependence for photodissociation of (NO) 2 + and (NO) 3 + and comparison of MPI spectra obtained with 266, 355, and 532 nm light indicate that the dissociation is occurring in the cluster ions.
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  • 32
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    The European physical journal 26 (1993), S. 267-269 
    ISSN: 1434-6079
    Keywords: 36.40 ; 73.20 ; 78.65 ; 82.65
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    Topics: Physics
    Notes: Abstract Collective and single electron excitations of large metal clusters supported on transparent substrates are investigated. The applied experimental techniques include extinction spectroscopy and laser induced dissociation accompanied by the ejection of individual atoms. The optical spectra depend on the electromagnetic far field and reflectcollective electron excitations of the conduction electrons, i.e. surface plasmons. Dissociation, however, is correlated to repulsivesingle electron energy levels. The characteristics of these localized excitations indicate a strong influence of collective excitations. In particular, it is found that nonlocal optical effects are important. In this picture surface plasmons catalytically enhance the number of single electron excitations and therefore of the metal atoms ejected as a result of the absorption of visible light. Results will be presented, which illustrate this interplay between collective and single electron excitations.
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  • 33
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    The European physical journal 26 (1993), S. 304-306 
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    Keywords: 36.40
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    Topics: Physics
    Notes: Abstract The phenomenon of surface melting in a Ni55 cluster is predicted from results of molecular dynamics simulations.
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  • 34
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    The European physical journal 26 (1993), S. 316-318 
    ISSN: 1434-6079
    Keywords: 36.40
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    Topics: Physics
    Notes: Abstract Structural and dynamical properties of gold clusters are derived from a Gupta-type potential using numerical simulations and are compared to features of nickel clusters derived from the same potential. The major implication of the comparison is that the properties of clusters mimicked by this many-body potential depend, in general, on the values of its parameters.
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  • 35
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    The European physical journal 26 (1993), S. 346-348 
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    Keywords: 36.40 ; 31.20.Sy
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    Topics: Physics
    Notes: Abstract We have investigated two generic structural models for Si clusters in the size range 20–33 atoms. The first model consists of stacks of puckered six-fold rings, with capping atoms on the two ends. The second model comprises compact structures with as many bulk-like four-fold coordinated atoms as possible. We have found the cohesive energy of the ring structures to be nearly constant as a function of cluster size, while that of the compact structures decreases dramatically with increasing size as more four-fold coordinated atoms are incorporated into the structures. We compare our results with recent experiments which suggest a crossover in stability between two cluster types in the size range studied here.
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  • 36
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    The European physical journal 26 (1993), S. 367-369 
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    Keywords: 36.40 ; 33.80
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    Topics: Physics
    Notes: Abstract Photoelectron spectra of (CO2)nH2O− (2≤n≤8) and (CO2)n(H2O) 2 − (1≤n≤2) were measured at the photon energy of 3.49 eV. The spectra show unresolved broad features, which are approximated by Gaussians. The vertical detachment energies (VDEs) were determined as a function of the cluster size. For (CO2)nH2O−, the VDE-n plots exhibit a sharp discontinuity between n=3 and 4; the VDE value is ≈3.5 eV at n=3, while it drops down abruptly to 2.59 eV at n=4. This discontinuity in VDE is ascribed to "core switching" at n=4; a C2O 4 − dimer anion forms the core of (CO2)nH2O− for n≤3, while a monomer CO 2 − is the core for n≥4. The (CO2)2(H2O) 2 − ion has a VDE of 2.33 eV, indicating the presence of a CO 2 − monomer core in the binary clusters containing two H2O molecules.
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  • 37
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    The European physical journal 26 (1993), S. 42-44 
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    Keywords: 36.40 ; 61.16.D ; 82.65.F
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    Topics: Physics
    Notes: Abstract We have madein-situ observation of electrodeposition on the graphite surface in electrolyte(0.5 mM-Bi2O3, 10 mM-HClO4) by means of Scanning Tunneling Microscopy(STM). We have observed the growth and the stripping of Bi metal particles of about 10 nm in diameter, with increase and decrease in the electrode potential, respectively. The STM images are taken in real time in a period of about 30 sec. They show that small particles grow in the initial stage, come in contact with each other, and coalesce in the contact area connecting two neighboring particles.
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  • 38
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    The European physical journal 26 (1993), S. 64-66 
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    Keywords: 36.40 ; 82.30
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    Topics: Physics
    Notes: Abstract The Pdn clusters are prepared by vapour deposition in an UHV chamber providing static secondary ion mass spectrometry (SSIMS) and thermo-programmed desorption analysis (TPD) facilities. By adjusting deposition parameters we are able to obtain isolated Pd species, dimers etc... In the present work we used as substrates thin films of γ-Alumina. We show that the reactivity and the kinetics of the CO-Pdn association depends on the cluster size.
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  • 39
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    The European physical journal 26 (1993), S. 115-117 
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    Keywords: 36.40
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    Topics: Physics
    Notes: Abstract Generating silver clusters by means of the gas aggregation technique, we have observed that in addition to larger clusters, a substantial amount of silver dimers is always present. This allows us to determine the vibrational population in the electronic ground state and, hence, the vibrational temperature of Ag2 optically. Temperatures between 70–300 K were measured in this experiment, dependent on cell parameters, e.g. evaporation rate, argon flow rate, length of the drift tube, etc. The high volume collisional rate of 1021 cm−3s−1 at the given pressures allows us to assume that the cluster temperature does not differ considerably from that of dimer.
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  • 40
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    The European physical journal 26 (1993), S. 156-158 
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    Keywords: 36.40
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    Topics: Physics
    Notes: Abstract Structures of small clusters of Ni, Pd, Pt, Cu, Ag, and Au with n=2−34 and n=55 atoms are calculated as functions of number of atoms and temperature by the simulated annealing Monte Carlo method using an embedded atom potential.
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  • 41
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    Keywords: 36.40 ; 82.20.Pm ; 82.30.Cf
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    Topics: Physics
    Notes: Abstract The development and characterization of a new fast-flow reactor for the study of the gas-phase chemical kinetics of small metal clusters is reported. The flow reactor has been designed to study the reactivity of well-thermalized clusters over a range of well-determined pressures in order to obtain quantitative absolute kinetic rate constants, especially in the low pressure limit. The apparatus has been characterized and proven through the study of known reactions of atoms and is capable of measuring bimolecular rate constants ranging five orders of magnitude down from gas kinetic at total pressures from 0.2 to 6 Torr. Application to the study of cluster kinetics has been demonstrated by measurements made on reactions of the copper dimer, Cu2.
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  • 42
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    The European physical journal 27 (1993), S. 89-92 
    ISSN: 1434-6079
    Keywords: 36.40 ; 61.50.C
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    Topics: Physics
    Notes: Abstract A simplified model for the calculation of the maximum possible cluster size in expanding nozzle flows, assuming a coagulation growth, is presented. For this model we assume seeded beams with lean mixtures, where the ratio of carrier gas pressure to vapour pressure is much larger than one. In this case the heat of condensation is effectively absorbed by the carrier gas. To estimate the maximum possible cluster size it is assumed that every collision of condensable material contributes to the cluster growth. The cluster sizeN, which is the number of monomers or atoms per cluster, is then given by the number of cluster-cluster collisionsZ N by the relation $$N = 2^{Z_N } $$ .
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  • 43
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    The European physical journal 26 (1993), S. 184-186 
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    Keywords: 36.40
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    Topics: Physics
    Notes: Abstract Photoelectron spectroscopy measurements of (NaCl)nNa− (n=1–13, except n=10) are reported. The observed electron energy spectra fall into three distinct types, reflecting different correlations between the two excess electrons and ions. Depending on the host clusters' structures, the experimental evidence indicates that the two excess electrons in these sodium chloride clusters could be spin paired, forming a bipolaron or a Na− anion. The two excess electrons could also be spin parallel, forming a double F-center state.
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  • 44
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    The European physical journal 26 (1993), S. 101-104 
    ISSN: 1434-6079
    Keywords: 36.40 ; 61.14.F ; 64.60.Q ; 82.20.M
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    Topics: Physics
    Notes: Abstract The significant advantages offered by systems of molecular clusters in the study of homogeneous nucleation are discussed. Determinations of nucleation rates in clusters can be followed experimentally in supersonic jets or computationally in molecular dynamics simulations. Extraordinarily high rates may be encountered, both in freezing and in solid-state transitions. From such information can be inferred the interfacial free energies, σsl and σSS, mechanisms of solid-state transitions. and an explanation of why certain crystalline phases not found in bulk systems can be seen in large molecular clusters.
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  • 45
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    The European physical journal 26 (1993), S. 28-32 
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    Keywords: 36.40
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    Topics: Physics
    Notes: Abstract The lattice gas Monte Carlo and tight binding method is used to study the electronic shell structure in large metallic clusters. The average density of states of a large ensemble of deformed clusters shows the same shell structure as the most spherical geometry. The level spacing distribution at the Fermi level is a Wigner distribution.
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  • 46
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    The European physical journal 26 (1993), S. 223-225 
    ISSN: 1434-6079
    Keywords: 36.40 ; 34.90
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    Topics: Physics
    Notes: Abstract Collision-induced reactions of size-selected cluster anions, (CO2) n − and (N2O)nO− with He and Kr atoms were studied at collision energies from 0.1 to 2.0 eV (center-of mass) by means of a tandem mass-spectrometer equipped with a pair of octapole ion guides. The dominant process was evaporation of the constituent molecules from the parent cluster ion. The absolute cross section for the evaporation was measured as functions of the size of the parent cluster ion and the collision energy. The reaction was explained by collisional excitation of the parent cluster ion followed by its unimolecular dissociation. The observed cross sections which correspond to those for the collisional excitation agree with those calculated in terms of charge-induced dipole and induced dipole-induced dipole interactions between the parent cluster ion and the target atom. The distributions of the product ions resulting from the unimolecular dissociation were reproduced by a simple calculation based on RRK theory. In the collision of (CO2) n − , the cross sections for (CO2) 10 − and (CO2) 14 − were significantly small and their abundances in the product ion distributions were particularly large. These findings indicate that (CO2) 10 − and (CO2) 14 − are stable species. On the other hand, stable species in (N2O)nO− was found to be (N2O)5O−.
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  • 47
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    The European physical journal 26 (1993), S. 45-47 
    ISSN: 1434-6079
    Keywords: 36.40 ; 64.70D
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    Topics: Physics
    Notes: Abstract We have studied the structural, dynamical and thermodynamical behaviour of Pb clusters in theN=147−2057 range, using a phenomenological many-body potential and molecular dynamics. Cuboctahedral structures, previously found to be particularly stable for this system, are used as starting configurations at lowT. Calculated size-dependent melting temperatures appear to be reasonably accounted for by Pawlow's law,T m (N)=T m (∞)−AN −1/3. The behaviour of the mean square displacements and direct structural observations suggest that melting initiates at the surface, in agreement with recent experimental observations. High-frequency surface peaks in the vibrational spectrum disappear asT approachesT m , in coincidence with the onset of surface diffusion.
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  • 48
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    The European physical journal 26 (1993), S. 82-86 
    ISSN: 1434-6079
    Keywords: 82.50 ; 36.40 ; 35.20.V
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    Topics: Physics
    Notes: Abstract Time-resolved observations of the fast electron transfer from an electron donor to metal ions adsorbed on metal clusters in solution have shown that a critical size of the cluster is required to make it capable of accepting electrons. The threshold is attributed to a size dependent redox potential of the cluster, increasing with the nuclearity (in contrast with the ionization potential in the gas phase which decreases when n increases): it corresponds to the nuclearity for which the cluster redox potential becomes more positive than the potential of the electron donor acting as a monitor. New data of redox potentials (or IP) of Agn clusters (hydroquinone as monitor) and Cun cluster (sulfonatopropylviologen anion as monitor) are derived. The influence of n and of the solvation or the ligand is discussed.
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  • 49
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    The European physical journal 26 (1993), S. 183-185 
    ISSN: 1434-6079
    Keywords: 36.40 ; 33.80 ; 35.20
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    Topics: Physics
    Notes: Abstract Supersonic jet expansions of mixtures of nitric oxide with either nitrous oxide or carbon dioxide have been investigated over a wide range of relative concentrations. Mixed molecular cluster ions of the form (NO) m + (N2O)n and (NO) m + (CO2)n are detected following non-resonant two-photon ionization. Over a wide range of intermediate concentrations, the cluster ion distributions (NO) 3 + (N2O)n and (NO) 3 + (CO2)n with n≤30 are significantly more intense than clusters containing other numbers of nitric oxide molecules. The extra abundance of these species is attributed to their especially stable structures and several possible forms are discussed. An intriguing possibility involves a stable cyclic nitric oxide trimer (or ion) when combined with nitrous oxide or carbon dioxide clusters.
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    The European physical journal 26 (1993), S. 216-218 
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    Keywords: 36.40
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    Topics: Physics
    Notes: Abstract A simple threshold electron analyzer was constructed and laser photodetachment threshold electron spectra of Si− and Si 4 − were measured.
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    The European physical journal 26 (1993), S. 252-254 
    ISSN: 1434-6079
    Keywords: 36.40
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    Topics: Physics
    Notes: Abstract Reactions of carbon clusterions with O2 were studied by using an RF ion trap in which cluster ions of specific size produced by laser ablation could be stored selectively. Reaction rate constants for positive and negative carbon cluster ions were estimated. In the case of the positive cluster ions, these were consistent with the previous experimental results using FTMS. Negative carbon cluster ions C n − (n=4−8) were much less reactive than positive cluster ions. The CnO− products were seen only in n=4 and 6.
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  • 52
    ISSN: 1434-6079
    Keywords: 36.40 ; 33.40.Hp ; 32.30.Bv
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    Topics: Physics
    Notes: Abstract A new metastable decay reaction of ArnO+ cluster ions produced by the electron impact ionization of argonoxygen clusters has been discovered, leading to the evaporation of more than two monomers in the metastable time regime. It is estimated that an energy of approx. 1 eV has to be released from the intramolecular to intermolecular modes prior to this metastable decay. In contrast to previously observed excimer-induced fragmentation of pure argon cluster ions, it has been concluded that the localized metastable state of an ionic rather than a neutral species is involved in the fragmentation. A reaction mechanism involving an electronic transition from the a2Π ArO+* (O(3P)-Ar+(2P)) excited state to the X4Σ− ArO+ (O+(4S)-Ar(1S)) ground state of the ArO+ complex ion within the cluster and subsequent release of considerable amount of vibrational energy to cluster modes is suggested to account for the observed fragmentation. Based on these measurements, a lifetime of approx. 2 µsis proposed for the excited state a2Π ArO+*.
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    The European physical journal 26 (1993), S. 338-340 
    ISSN: 1434-6079
    Keywords: 35.20 ; 36.40
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    Topics: Physics
    Notes: Abstract Temperature effects on heat capacity in four and three component systems N2O-HCN and CO-C2H2, respectively, were computed. Structural and vibrational parameters originated from the second order Møller-Plesset perturbation treatment with the 6-31++G** basis set while relative energies were of a still advanced nature. Isomerism contribution to heat capacity exhibits two temperature maxima at 43 and 205 or 15 and 83 K in N2O-HCN or CO-C2H2. The highest reported isomeric enhancement of the total heat capacity is about 27 %.
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  • 54
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    The European physical journal 28 (1993), S. 169-175 
    ISSN: 1434-6079
    Keywords: 42.65.K ; 36.40 ; 73.35
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    Topics: Physics
    Notes: Abstract We calculate the nonlinear optical properties of small metallic spheres using electromagnetic theory and assuming that the local response of the conduction electrons is the same as for a plane surface. Electromagnetic Mie-resonances cause a strong increase of the second and higher harmonics in the reflected light. Detailed results are given for the second and third harmonic generation, its dependence on the frequency and polarization of the incident light, and on the cluster size. An enhancement of the second harmonic generation by a factor of about 5000 is obtained for small spherical metallic clusters. This is in good agreement with experiments on artificially roughened metal surfaces.
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    The European physical journal 28 (1993), S. 235-245 
    ISSN: 1434-6079
    Keywords: 36.40 ; 35.20.Wg ; 71.45.Nt
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    Topics: Physics
    Notes: Abstract We propose a modified Nilsson model for spheroidal sodium clusters and investigate the modification of shell structure by deformation for sizes up toN=850. For spherical clusters, our potential is fitted to the single-particle spectra obtained from microscopically selfconsistent Kohn-Sham calculations using the jellium model and the local density approximation. Employing Strutinsky's shell-correction method, the surface energy of the jellium model is renormalized to its experimental value. We find good agreement between our theoretically predicted deformed magic numbers and the experimentally observed ones extracted from recent sodium mass abundance spectra.
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