Stability effects of AunXm+ (X=Cu, Al, Y, In) clusters

Bouwen, Wim; Vanhoutte, Frederik; Despa, Florin; Bouckaert, Steven; Neukermans, Sven; Kuhn, Luise Theil; Weidele, H.; Lievens, Peter; Silverans, Roger

doi:10.1016/s0009-2614(99)01150-1

Cited by 133 publications

(97 citation statements)

References 33 publications

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“…The change of the cluster potential may, in turn, alter the ordering of the related electron shells, a fact which has been observed in many experiments. [30][31][32] Therefore our findings may be interpreted as qualitative support for various models explaining the shell inversions for doped metallic clusters. [38][39][40][41] Obviously other kinds of changes of dopant atoms may induce still different effects, that will depend on their locations in the cluster.…”

supporting

confidence: 81%

“…This analysis is important in the context of recent observations of the role played by composition and geometry in changing the physical properties of metallic clusters. [30][31][32] Consider a fixed positive ion distribution in space r + (R i ), with R i the positions of the ions measured from the center of the cluster. The ion cluster cage has a net charge measured in appropriate units equal to zN, where z is the electric charge of one ion (for simplicity, we shall restrict the discussion to single-valent metals, z ¼ 1) and N denotes the total number of ions in the cluster.…”

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confidence: 99%

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Visualization of the effective potential and Coulomb correlations in finite metallic systems

Despa

Berry

2002

Phys. Chem. Chem. Phys.

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We present an analytic ansatz to find the effective electrostatic potential and Coulomb correlations in multicenter problems, specifically homogeneous and doped clusters of metal atoms. The approach is based on a quasi-classical density-functional treatment. We focus on the interpretive aspect of our findings, particularly on extracting insight regarding the geometric effects of Coulomb correlations for any given spatial disposition of ionic cores. For singly-doped metallic clusters we obtain a direct visualization of the variations of both screening and Coulomb correlations with changes of location of the dopant atom. This analysis provides a way to interpret recent observations of the variability of physical properties of metal clusters with changes of composition and geometry.Perception in terms of concepts that can be visualized is an important part of understanding physical phenomena. Presently, such an interpretative theoretical tool may provide a valuable way of guiding the analysis of experiment in the realm of atomic clusters. Hence, we develop an analytic approach that makes it possible to find and visualize the effective electrostatic potential and Coulomb correlations in multicenter problems. We make use of the quasi-classical density-functional theory to account for the electron self-distribution in the common cluster potential. While this is not at the same level of studies of electron correlations in atoms, for which very accurate wave functions have been used, it is a significant step beyond the '' jellium '' model, frequently-invoked in describing moderately large metallic clusters. Collective effects induced by Coulomb correlations in atoms have been studied in two ways. In the first, both hydrodynamic theory and local approximate dielectric theory have been used; neither of these takes into account either shell structure or the single-particle spectrum of the valence electrons.2 These methods are capable, at most, of giving gross trends in dynamical properties. The second route instead uses a fully quantal description based on the one-electron excitation spectrum and corresponding wavefunctions. A recent collection of papers provides a description of methods and results of the application of many-body techniques in atomic theory. The way electrons are correlated can be inferred from the probability distribution implied by their wavefunction. 4 To make such inferences, however, we must be a bit thoughtful about how we present this distribution. Even for a two-electron atom, we begin with a function of six independent variables in a fixed-center-of-mass system. We would like to extract from this a description in no more than two or three independent variables, something we can represent pictorially and visualize.For a three-body system such as He** or the valence electrons of Mg, a natural and practical way to carry out such a description has emerged as an analytic reduction of the probability density |C(r 1 ,r 2 )| 2 to the joint probability density p(r 1 ,r 2 ,y 12 ), where y 12 is the angle b...

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confidence: 81%

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confidence: 99%

Visualization of the effective potential and Coulomb correlations in finite metallic systems

Despa

Berry

2002

Phys. Chem. Chem. Phys.

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“…Previous studies have shown that even-numbered neutral silver clusters show enhanced chemical stability due to electron pairing. Meanwhile, for charged clusters, electron pairing occurs when they consist of odd numbers of atoms (Yannouleas and Landman 1995;Bouwen et al 1999;Schmidt et al 2003;Peineke et al 2009). Higher chemical stability leads to lower sensitivity to impurities and thus, more abundance in the measured distributions.…”

Section: Results and Discussion Silver Cluster: Identification Of Clumentioning

confidence: 99%

Atomic Cluster Generation with an Atmospheric Pressure Spark Discharge Generator

Maisser

Barmpounis

Attoui

et al. 2015

Aerosol Science and Technology

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A new method for generating metal clusters in the gas phase is described and characterized in this work. The method is based on material evaporation by spark ablation at atmospheric pressure. The characterization of atomic clusters was done by measuring their electrical mobility. The measured mobilities were compared with values found in literature in order to identify the cluster species. We show that silver clusters consisting from one up to 25 atoms can be produced in helium at atmospheric pressure. In addition, the effect of oxygen concentration on the resulting cluster mobility distribution was investigated. Results show that at higher oxygen level, the mobility distribution is dominated by the abundance of stable clusters (i.e., magic number clusters). This can be attributed to an oxidation etching effect.

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“…This finding is consistent with previous photofragmentation experiments on Au n−1 Cu + yielding equivalent stability patterns as Au n + , which already indicated a nearly unaltered geometrical structure upon Cu doping. 43 On the other hand, a recent photoelectron spectroscopy study on anionic clusters demonstrated a shift of the 2D → 3D structural transition from Au 12 − to Au 10 M − upon isolectronic substitution with M = Cu and Ag. 44 Also calculations on neutral Au n−1 Cu using the semi-empirical Gupta potential and a genetic algorithm predicted a considerable change in the geometry by the mere substitution of Au by Cu.…”

Section: Geometrical Structure Of Copper Doped Gold Clustersmentioning

confidence: 99%

Copper doping of small gold cluster cations: Influence on geometric and electronic structure

Lang

Claes

Cuong

et al. 2011

The Journal of Chemical Physics

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Analytical approach for the excited-state Hessian in time-dependent density functional theory: Formalism, implementation, and performance J. Chem. Phys. 135, 184111 (2011) Stability analysis of multiple nonequilibrium fixed points in self-consistent electron transport calculations J. Chem. Phys. 135, 174111 (2011) Communication: Orbital instabilities and triplet states from time-dependent density functional theory and longrange corrected functionals J. Chem. Phys. 135, 151103 (2011) All-electron time-dependent density functional theory with finite elements: Time-propagation approach J. Chem. Phys. 135, 154104 (2011) Additional information on J. Chem. Phys. The effect of Cu doping on the properties of small gold cluster cations is investigated in a joint experimental and theoretical study. Temperature-dependent Ar tagging of the clusters serves as a structural probe and indicates no significant alteration of the geometry of Au n + (n = 1-16) upon Cu doping. Experimental cluster-argon bond dissociation energies are derived as a function of cluster size from equilibrium mass spectra and are in the 0.10-0.25 eV range. Near-UV and visible light photodissociation spectroscopy is employed in conjunction with time-dependent density functional theory calculations to study the electronic absorption spectra of Au 4-m Cu m + (m = 0, 1, 2) and their Ar complexes in the 2.00−3.30 eV range and to assign their fragmentation pathways. The tetramers Au 4 + , Au 4 + · Ar, Au 3 Cu + , and Au 3 Cu + · Ar exhibit distinct optical absorption features revealing a pronounced shift of electronic excitations to larger photon energies upon substitution of Au by Cu atoms. The calculated electronic excitation spectra and an analysis of the character of the optical transitions provide detailed insight into the composition-dependent evolution of the electronic structure of the clusters.

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Stability effects of AunXm+ (X=Cu, Al, Y, In) clusters

Cited by 133 publications

References 33 publications

Visualization of the effective potential and Coulomb correlations in finite metallic systems

Visualization of the effective potential and Coulomb correlations in finite metallic systems

Atomic Cluster Generation with an Atmospheric Pressure Spark Discharge Generator

Copper doping of small gold cluster cations: Influence on geometric and electronic structure

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