A diffusion Monte Carlo study of small para-Hydrogen clusters

Ground state energies and chemical potentials of parahydrogen clusters are calculated from 3 to 40 molecules using the diffusion Monte Carlo technique with two different pH2-pH2 interactions. This calculation improves a previous one by the inclusion of three-body correlations in the importance sampling, by the time step adjustement and by a better estimation of the statistical errors. Apart from the cluster with 13 molecules, no other magic clusters are predicted, in contrast with path integral Monte Carlo results

Close-Packing of Clusters: Application to Al_100

The lowest energy configurations of close-packed clusters up to N=110 atoms with stacking faults are studied using the Monte Carlo method with Metropolis algorithm. Two types of contact interactions, a pair-potential and a many-atom interaction, are used. Enhanced stability is shown for N=12, 26, 38, 50, 59, 61, 68, 75, 79, 86, 100 and 102, of which only the sizes 38, 75, 79, 86, and 102 are pure FCC clusters, the others having stacking faults. A connection between the model potential and density functional calculations is studied in the case of Al_100. The density functional calculations are consistent with the experimental fact that there exist epitaxially grown FCC clusters starting from relatively small cluster sizes. Calculations also show that several other close-packed motifs existwith comparable total energies.Comment: 9 pages, 7 figure

Size-dependent melting: Numerical calculations of the phonon spectrum

In order to clarify the relationship between the phonon spectra of nanoparticles and their melting temperature, we studied in detail the size-dependent low energy vibration modes. A minimum model with atoms on a lattice and harmonic potentials for neighboring atoms is used to reveal a general behavior. By calculating the phonon spectra for a series of nanoparticles of two lattice types in different sizes, we found that density of low energy modes increases as the size of nanoparticles decreases, and this density increasing causes decreasing of melting temperature. Size-dependent behavior of the phonon spectra accounts for typical properties of surface-premelting and irregular melting temperature on fine scales. These results show that our minimum model captures main physics of nanoparticles. Therefore, more physical characteristics for nanoparticles of certain types can be given by phonons and microscopic potential models.Comment: 5 pages, 5 figure

Growth of epitaxially oriented Ag nanoislands on air-oxidized Si(111)-(7x7) surfaces: Influence of short range order on the substrate

Clean Si(111)-(7{x7) surfaces, followed by air-exposure, have been investigated by reflection high energy electron diffraction (RHEED) and scanning tunneling microscopy (STM). Fourier transforms (FTs) of STM images show the presence of short range (7x7) order on the air-oxidized surface. Comparison with FTs of STM images from a clean Si(111)-(7x7) surface shows that only the 1/7th order spots are present on the air-oxidized surface. The oxide layer is ~ 2-3 nm thick, as revealed by cross-sectional transmission electron microscopy (XTEM). Growth of Ag islands on these air-oxidized Si(111)-(7x7) surfaces has been investigated by in-situ RHEED and STM and ex-situ XTEM and scanning electron microscopy. Ag deposition at room temperature leads to the growth of randomly oriented Ag islands while preferred orientation evolves when Ag is deposited at higher substrate temperatures. For deposition at 550{\deg}C face centered cubic Ag nanoislands grow with a predominant epitaxial orientation [1 -1 0]Ag || [1 -1 0]Si, (111)Ag || (111)Si along with its twin [-1 1 0]Ag || [1 -1 0]Si, (111)Ag || (111)Si, as observed for epitaxial growth of Ag on Si(111) surfaces. The twins are thus rotated by a 180{\deg} rotation of the Ag unit cell about the Si [111] axis. It is intriguing that Ag nanoislands follow an epitaxial relationship with the Si(111) substrate in spite of the presence of a 2-3 nm thick oxide layer between Ag and Si. Apparently the short range order on the oxide surface influences the crystallographic orientation of the Ag nanoislands.Comment: 10 figure

Surface structure and solidification morphology of aluminum nanoclusters

Classical molecular dynamics simulation with embedded atom method potential had been performed to investigate the surface structure and solidification morphology of aluminum nanoclusters Aln (n = 256, 604, 1220 and 2048). It is found that Al cluster surfaces are comprised of (111) and (001) crystal planes. (110) crystal plane is not found on Al cluster surfaces in our simulation. On the surfaces of smaller Al clusters (n = 256 and 604), (111) crystal planes are dominant. On larger Al clusters (n = 1220 and 2048), (111) planes are still dominant but (001) planes can not be neglected. Atomic density on cluster (111)/(001) surface is smaller/larger than the corresponding value on bulk surface. Computational analysis on total surface area and surface energies indicates that the total surface energy of an ideal Al nanocluster has the minimum value when (001) planes occupy 25% of the total surface area. We predict that a melted Al cluster will be a truncated octahedron after equilibrium solidification.Comment: 22 pages, 6 figures, 34 reference

Molecular dynamics simulations of lead clusters

Molecular dynamics simulations of nanometer-sized lead clusters have been performed using the Lim, Ong and Ercolessi glue potential (Surf. Sci. {\bf 269/270}, 1109 (1992)). The binding energies of clusters forming crystalline (fcc), decahedron and icosahedron structures are compared, showing that fcc cuboctahedra are the most energetically favoured of these polyhedral model structures. However, simulations of the freezing of liquid droplets produced a characteristic form of ``shaved'' icosahedron, in which atoms are absent at the edges and apexes of the polyhedron. This arrangement is energetically favoured for 600-4000 atom clusters. Larger clusters favour crystalline structures. Indeed, simulated freezing of a 6525-atom liquid droplet produced an imperfect fcc Wulff particle, containing a number of parallel stacking faults. The effects of temperature on the preferred structure of crystalline clusters below the melting point have been considered. The implications of these results for the interpretation of experimental data is discussed.Comment: 11 pages, 18 figues, new section added and one figure added, other minor changes for publicatio

Hierarchical self-assembly of Au-nanoparticles into filaments: evolution and break

We compare the assembly of individual Au nanoparticles in a vacuum and between two Au(111) surfaces via classical molecular dynamics on a timescale of 100 ns. In a vacuum, the assembly of three nanoparticles used as seeds, initially showing decahedral, truncated octahedral and icosahedral shapes with a diameter of 1.5–1.7 nm, evolves into a spherical object with about 10–12 layers and a gyration radius ∼2.5–2.8 nm. In a vacuum, 42% show just one 5-fold symmetry axis, 33% adopt a defected icosahedral arrangement, and 25% lose all 5-fold symmetry and display a face-centred-cubic shape with several parallel stacking faults. We model a constrained version of the same assembly that takes place between two Au(111) surfaces. During the dynamics, the two Au(111) surfaces are kept fixed at distances of 55 Å, 55.5 Å, 56 Å, and 56.5 Å. The latter distance accommodates 24 Au layers with no strain, while the others correspond to nominal strains of 1.5%, 2.4%, and 3.3%, respectively. In the constrained assembly, each individual seed tends to reorganize into a layered configuration, but the filament may break. The probability of breaking the assembled nanofilament depends on the individual morphology of the seeds. It is more likely to break at the decahedron/icosahedron interface, whilst it is more likely to layer with respect to the (111) orientation when a truncated octahedron sits between the decahedron and the icosahedron. We further observe that nanofilaments between surfaces at 56 Å have a >90% probability of breaking, which decreases to 8% when the surfaces are 55 Å apart. We attribute the dramatic change in probability of breaking to the peculiar decahedron/icosahedron interface and the higher average atomic strain in the nanofilaments. This in silico experiment can shed light on the understanding and control of the formation of metallic nanowires and nanoparticle-assembled networks, which find applications in next-generation electronic devices, such as resistive random access memories and neuromorphic devices