Shaun C. Hendy

Light Scattering in Transparent Glass Ceramics

Transparent glass ceramic materials, with microstructures comprised of dispersed nanocrystallites in a residual glass matrix, offer the prospect of nonlinear optical properties. However, good transparency requires low optical scattering and low atomic absorption. The attenuation of light due to scattering (turbidity) will depend upon the difference in refractive index of the two phases and the size and distribution of crystals in the glass. Here, we model the glass ceramic as a late-stage phase-separated structure, and compute scattering in this model. We find that the turbidity follows a k8R7 relationship, where k is the wave vector of light in the glass ceramic and R is the average radius of the crystals in the glass.

Real-Time TEM and Kinetic Monte Carlo Studies of the Coalescence of Decahedral Gold Nanoparticles

We report on a real-time in situ TEM study of the coalescence of individual pairs of decahedral gold nanoparticles, which have been synthesized in solution. We observe the rate of growth of the neck that joins two particles during coalescence and compare this to classical continuum theory and to atomistic kinetic Monte Carlo simulations. We find good agreement between the observations and the simulations but not with the classical continuum model. This disagreement is attributed to the faceted nature of the particles.

Coalescence of nanoscale metal clusters: Molecular-dynamics study

We study the coalescence of nanoscale metal clusters in an inert-gas atmosphere using constant-energy molecular dynamics. The coalescence proceeds via atomic diffusion with the release of surface energy raising the temperature. If the temperature exceeds the melting point of the coalesced cluster, a molten droplet forms. If the temperature falls between the melting point of the larger cluster and those of the smaller clusters, a metastable molten droplet forms and freezes.

Capillary absorption of metal nanodroplets by single-wall carbon nanotubes.

We present a simple model that demonstrates the possibility of capillary absorption of nonwetting liquid nanoparticles by carbon nanotubes (CNTs) assisted by the action of the Laplace pressure due to the droplet surface tension. We test this model with molecular dynamics simulation and find excellent agreement with the theory, which shows that for a given nanotube radius there is a critical size below which a metal droplet will be absorbed. The model also explains recent observations of capillary absorption of nonwetting Cu nanodroplets by carbon nanotubes. This finding has implications for our understanding of the growth of CNTs from metal catalyst particles and suggests new methods for fabricating composite metal-CNT materials.

Molecular dynamics simulations of reflection and adhesion behavior in Lennard-Jones cluster deposition

We conduct molecular dynamics simulations of the collision of atomic clusters with a weakly attractive surface. We focus on an intermediate regime, between soft landing and fragmentation, where the cluster undergoes deformation on impact but remains largely intact and will either adhere to the surface (and possibly slide) or be reflected. We find that the outcome of the collision is determined by the Weber number We, i.e., the ratio of the kinetic energy to the adhesion energy, with a transition between adhesion and reflection occurring as We passes through unity. We also identify two distinct collision regimes: in one regime, the collision is largely elastic and deformation of the cluster is relatively small, but in the second regime, the deformation is large and the adhesion energy starts to depend on the kinetic energy. If the transition between these two regimes occurs at a similar kinetic energy to that of the transition between reflection and adhesion, then we find that the probability of adhesion for a cluster can be bimodal. In addition, we investigate the effects of the angle of incidence on adhesion and reflection. Finally, we compare our findings both with recent experimental results and with macroscopic theories of particle collisions.

Superheating and solid-liquid phase coexistence in nanoparticles with nonmelting surfaces.

We present a phenomenological model of melting in nanoparticles with facets that are only partially wet by their liquid phase. We show that in this model, as the solid nanoparticle seeks to avoid coexistence with the liquid, the microcanonical melting temperature can exceed the bulk melting point and that the onset of coexistence is a first-order transition. We show that these results are consistent with molecular dynamics simulations of aluminum nanoparticles which remain solid above the bulk melting temperature.

Transition from Icosahedral to Decahedral Structure in a Coexisting Solid-Liquid Nickel Cluster

We have used molecular dynamics simulations to construct a microcanonical caloric curve for a 1415 atom Ni icosahedron. Prior to melting, the Ni cluster exhibits static solid-liquid phase coexistence. Initially, a partial icosahedral structure coexists with a partially wetting melt. However, at energies very close to the melting point the icosahedral structure is replaced by a truncated decahedral structure that is almost fully wet by the melt. This structure remains until the cluster fully melts. The transition appears to be driven by a preference for the melt to wet the decahedral structure.

Surface-reconstructed icosahedral structures for lead clusters

We describe a family of icosahedral structures for lead clusters. In general, structures in this family contain a Mackay icosahedral core with a reconstructed two-shell outer-layer. This family includes the anti-Mackay icosahedra, which has a Mackay icosahedral core but with most of the surface atoms in hexagonal close-packed positions. Using a many-body glue potential for lead, we identify two icosahedral structures in this family which have the lowest energies of any known structure in the size range from 900 to 15 000 lead atoms. We show that these structures are stabilized by a feature of the many-body glue part of the interatomic potential.

Solid-liquid phase coexistence and structural transitions in palladium clusters

We use molecular dynamics with an embedded atom potential to study the behavior of palladium nanoclusters near the melting point in the microcanonical ensemble. We see transitions from both fcc and decahedral ground state structures to icosahedral structures prior to melting over a range of cluster sizes. In all cases this transition occurs during solid-liquid phase coexistence and the mechanism for the transition appears to be fluctuations in the molten fraction of the cluster and subsequent recrystallization into the icosahedral structure.

Effect of patterned slip on micro- and nanofluidic flows

We consider the flow of a Newtonian fluid in a nano- or microchannel with walls that have patterned variations in slip length. We formulate a set of equations to describe the effects on an incompressible Newtonian flow of small variations in slip and solve these equations for slow flows. We test these equations using molecular dynamics simulations of flow between two walls which have patterned variations in wettability. Good qualitative agreement and a reasonable degree of quantitative agreement is found between the theory and molecular dynamics simulations. The results of both analyses show that patterned wettability can be used to induce complex variations in flow. Finally we discuss the implications of our results for the design of microfluidic mixers using slip.