Preferred structures of the atomic Ag islands on silicone oil surfaces

Varying the substrate temperature T(s) from 285 to 353 K, both the aggregation behavior of Ag atoms and the preferred structures of the atomic Ag islands on silicone oil surfaces are investigated. After deposition, the deposited Ag atoms form isolated islands with a preferred height. Our observations reveal that, as T(s) increases, the preferred island height increases from 20.0 to 33.0 nm, which results in the decrease of the Ag apparent coverage, from 9.6 ± 0.1% to 6.5 ± 0.3%. Further, the crystal structure of the Ag islands changes from amorphous to polycrystalline as the substrate temperature T(s) goes up. Subsequently a 3D aggregation mechanism of the Ag atoms on the liquid substrates is proposed.     

Magnetism of Fe clusters and islands on Pt surfaces

Clusters and islands of Fe atoms have been prepared by noble gas buffer layer assisted growth as well as by standard molecular beam epitaxy on Pt substrates. Xe buffer layers have been utilized to promote the formation of compact, relaxed Fe clusters with narrow size distribution. Without the Xe buffer, strained Fe islands with a characteristic misfit dislocation network are formed. Magnetization loops obtained by magneto-optical Kerr effect measurements reveal that in-plane easy magnetization axis is only found for the relaxed clusters, pointing out the important role of epitaxial lattice deformations for the magnetic anisotropy. PACS 61.46.+w; 68.37.Ef; 36.40.Cg; 75.75.+a     

Morphology and microstructure of Ag islands of aggregated atoms on oil surfaces

The morphology evolution of silver islands on silicone oil surfaces is measured and the microstructure of the islands is studied. The deposited Ag atoms diffuse and aggregate on the oil surface and then Ag islands with the width of the order of 102-nm form. After the samples are removed from the vacuum chamber, the immediate measurement shows that the apparent Ag coverage of the total area decays with the magnitude up to (23.0±3.8)% in few minutes. In the following two hours, the samples are kept in the ambient atmosphere and several unexpected results are detected: 1) as the topological structure of the islands evolves, the total area of each island decreases gradually and the maximum decrement measured is around 20%; 2) if an island breaks and becomes two small pieces, the total area decreases obviously; 3) however, if two small islands meet and stick together, a sudden increment of the total area is observed. These phenomena, mirroring the evolution process of the island microstructure, are resulted from both the diffusion of the atoms and the combination of the defects inside the islands.     

Shallow implantation of "Size-Selected" Ag clusters into graphite

We have investigated the implantation of Ag(N) (N = 20-200) clusters into a graphite substrate over the range of energies (E) 0.75-6 keV using molecular dynamics simulations. We find that after implantation the silver clusters remain coherent, albeit amorphous, and rest at the bottom of an open tunnel in the graphite created by the impact. It is found that the implantation depth of the clusters varies linearly as E/N2/3. We conclude that the cluster is decelerated by a constant force proportional to its cross-sectional area. We also identify a threshold energy for surface penetration associated with elastic compression of the graphite substrate.     

Si(001)表面硅氧团簇原子与电子结构的第一性原理研究

在周期性边界条件下的k空间中,采用基于密度泛函理论的第一性原理广义梯度近似方法,对建立的规则对称型结构（A）、周期性非对称型结构（B）、周期性非对称型结构（C）、不规则型结构（D）四种可能的Si（001）表面硅氧团簇的结构模型进行了优化计算.结果表明优化后的表面结构呈无定形状,并且优化后的B,C,D三种模型的表面结构具有类似SiO₂的四面体结构的几何特征.此外,通过电子局域函数图以及Mulliken布居分析发现硅氧团簇中的Si—O键既有明显的离子键成分,也有一定的共价键成分. 关键词： Si（001）表面 硅氧团簇 密度泛函理论 第一性原理     

Strong influence of defects on the electronic structure of Pt adatoms and clusters on graphite

We study the specific impact of defects such as step edges at the graphite surface on the electronic configuration of adsorbed Pt atoms and Pt₈ clusters. Surface diffusion is strongly reduced by depositing Pt and Pt₈ into a thin rare gas layer. In this configuration a very narrow adatom Pt 4f spectrum is found at an exceptionally small binding energy, similar to Pt surfaces. Both, adatom and cluster spectra are strongly shifted towards higher binding energy when allowed to diffuse towards defects like step edges. The strong shifts are indicative of a chemical reaction at the step edges and are conjectured to be part of the particle size dependent binding energy shifts typically observed for transition metal clusters grown on the surface of graphite.     

Scanning tunnelling microscopy and electronic structure of Mn clusters on Ag(111)

Small Mn clusters (Mn₁-Mn₄) are prepared by manipulation of Mn adatoms on Ag(111) with the tip of a scanning tunnelling microscope. The apparent heights of the clusters are observed to increase monotonously from 1.6 Å for a monomer to 2.2 Å for a tetramer. Self-consistent calculations of the electronic structure of these clusters are in encouraging agreement with the experimental data.     

Coarsening of mass-selected Au clusters on amorphous carbon at room temperature

Low-energy cluster beam deposition was used to deposit mass-selected Au_n clusters (n = 4, 6, 13 and 20) on amorphous carbon (a-C) substrates. The resulting samples were stored at room temperature under ambient conditions for time periods up to 32 months to analyze the coarsening behaviour of the clusters. Cluster-size distributions were measured in regular time intervals by transmission electron microscopy (TEM). The TEM experiments show a significant increase of the average cluster size with time analogous to classical surface Ostwald ripening (OR). The coarsening of Au clusters can be well described by steady-state diffusion-limited kinetics. The derived surface mass-transport diffusion coefficients at room temperature range between 1.1 and 3.8·10⁻²⁵ m² s⁻¹ for our samples. A detailed analysis of values suggests that, the rate of the surface OR for mass-selected Au_n clusters increases with the cluster size in the sequence: Au₄ ≈ Au₆ < Au₁₃ < Au₂₀ for the investigated range of Au clusters. Given that the initial, on-surface cluster-size distributions are nominally monodisperse, classical OR with cluster coarsening based only on the Gibbs-Thomson effect cannot explain the observed coarsening. The activation of the coarsening process is rationalized by initial variations of the cluster sizes due to the deposition process itself and/or the interaction of the clusters with the substrate. Moreover, the presence of initial deposited Au clusters as different isomers with slightly different chemical potential on the substrate, may also initiate the coarsening by surface OR. Furthermore, we find that the coarsening is most pronounced for the paucidispersed sample with Au_m (10 ? m ? 20) clusters. A possible explanation of this behaviour is the presence of an initial distribution of different cluster sizes directly after deposition.     

Deposition and diffusion of size-selected (Ag400+) clusters on a stepped graphite surface

400 clusters on a stepped graphite surface by a combination of scanning electron microscopy experiments and computer simulations (molecular dynamics and Monte Carlo methods). We find that the shape of the clusters is only partially deformed by the impact with the surface, moreover the clusters do not create surface defects upon landing, and so are able to diffuse freely over the surface. Many clusters are found to become trapped at surface steps, where their mobility is reduced by the higher binding energy. Exploring the 1-D diffusion of clusters along the steps reveals the low mobility for larger islands, as well as the importance of defects on the step (for example kinks), which trap the mobile clusters. Received: 9 April 1998/Accepted: 25 August 1998     

First-principles study of structures and electronic properties of cadmium sulfide clusters

The lowest-energy structures and the electronic properties of CdnSn （n = 1 - 8） clusters have been studied by using denslty-functional theory simulating package DMol^3 in the generalized gradient approximation （GGA）. The ring-like structures are the lowest-energy configurations for n = 2, 3 and the three-dimensional spheroid configurations for n = 4 - 8. The three-dimensional structures may be considered as being built from the Cd2S2 and Cd3S3 rings. Compared to the previous reports, we have found the more stable structures for CdnSn（n = 7, 8）. Calculations show that the magic numbers of CdnSn （n = 1-8） clusters are n = 3 and 6. As cluster size increases, the properties of CdnSn clusters tend to bulk-like ones in binding energy per CdS unit and Mulliken atomic charge, obtained by comparing with the calculated results of the wurtzite and zinc blende CdS for the same simulating parameters.     

金团簇结构和电子性质的密度泛函研究

采用密度泛函理论,研究了Aun(2≤n≤10)团簇的最优结构和电子性质.采用各种不同的拓扑结构进行优化,计算结果显示最优结构都是二维的;在得到的最优结构基础上,进一步研究了其电子性质.结合能的二阶差分,费米能和能隙都显示了奇偶谐振效应.具有偶数个原子的金团簇要比奇数个原子的金团簇稳定,这与金团簇中的电子配对紧密相关.     

Scaling relations for implantation of size-selected Au,Ag, and Si clusters into graphite

The deposition of size-selected clusters represents a new route to the fabrication of truly nanometer-scale surface architectures, e.g., nanopores. We report a systematic experimental study, coupled with molecular dynamics simulations, of the implantation depths of size-selected Au7, Ag7, and Si7 clusters in the model graphite substrate. For impact energies between 1.0 and 5.5 keV, we find that the implantation depth scales linearly with the momentum of the clusters for all three types of cluster. This "universal" behavior is consistent with a (viscous) retarding force proportional to the velocity of the cluster, akin to Stokes's law.     

Collective electronic excitations in clusters in the vicinity of metal surfaces

We study the collective excitations of metal clusters approaching a metal surface. Using a simple model for the frequency-dependent dielectric constant ε(ω) and the multiple scattering method, we numerically investigate the shift in the plasmon resonance due to the coupling of the collective modes of the sphere with those of its mirror image. Results of the model calculation are verified by means of ab initio theory. As a prototype system we study Na₉ ⁺ cluster on the Cu(100) surface. The representation of the solid surface by a cluster of several, typically 54 substrate atoms, is used in combination with a high level configuration interaction (CI) calculation. PACS 31.15.Dv; 36.40.Gk; 73.20.-f     

Au-Pd与Au-Pt合金团簇稳定结构对比

由贵金属元素组成的合金团簇在光、电、磁和催化等领域吸引了广泛的研究兴趣.本文基于多体Gupta势函数采用内核构建的自适应免疫优化算法优化了Au-Pd和Au-Pt团簇最稳定结构.研究结果显示98原子Au-Pd与Au-Pt团簇均包含面心立方结构、十面体、二十面体和Leary四面体结构,但是两者的构型分布上存在着差异.键数变化分析结果显示Au原子分布趋势接近.此外,147原子Au-Pd和AuPt团簇均为完整二十面体结构.序列参数分析显示均形成核层结构.