RESUMEN
Several first-principles surface and bulk electronic structure calculations relating to the nucleation and growth of single-wall carbon nanotubes are described. Density-functional theory in various forms is used throughout. In the surface-related calculations, a 38-atom Ni cluster and several low-index Ni surfaces are investigated using pseudopotentials and plane-wave expansions. The energetic ordering of the sites for C atom adsorption is found to be the same, with the Ni(100) facet favored. The bulk diffusion coefficient of C in Ni as a function of cluster size and temperature is calculated from various molecular dynamics approaches. In another group of bulk-related calculations, Gaussian orbital basis sets are used to study a cluster or "flake" containing 14 C atoms. The flake is a segment of three hexagons from an "unrolled" carbon nanotube, with an armchair termination. The binding energies of C, Ni, Co, Fe, Cu, and Au atoms to it were calculated in an effort to gain insight into the mechanism for the high catalytic activity of Ni, Co, and Fe and the lack of it in Cu and Au. The binding energies of Cu and Au are about 1 eV less than those of the three catalytic elements. Similar methods are used to study the initial stages of nanotube growth within the context of classical nucleation theory. Finally, issues relating to the establishment of a fundamental catalytic mechanism are addressed.
Asunto(s)
Electrones , Nanotubos de Carbono/química , Adsorción , Carbono/química , Catálisis , Metales , Modelos Químicos , Níquel/química , Distribución Normal , Temperatura , Termodinámica , Factores de TiempoRESUMEN
We report the observation of 3D linear or branched chains of polymer-blend microspheres generated from liquid droplets of solution where the modified surface structure of the polymer composite results in highly robust interparticle bonds. Using a linear quadrupole to precisely position particles in space, we are able to take advantage of this novel material property to actively assemble particles in programmable three-dimensional architectures. The robust interlocking nature of interparticle linkage gives rise to strongly coupled morphology-dependent resonances in bisphere and trisphere systems, suggesting the possibility of three-dimensional photonic "molecules" and microscale optical manipulation applications.
RESUMEN
We report a new kind of photonic wire structure made from the sequential attachment of polymer-blend microparticles. Using a linear quadrupole to manipulate the particles in space, we are able to take advantage of a modified surface structure in the blend particle to actively assemble particles in programmable two- or three-dimensional architectures. Strong resonance features in fluorescence are observed near the intersection of linked spheres that cannot be interpreted with a two-dimensional (equatorial plane) model. Three-dimensional ray optics calculations show long-lived periodic trajectories that propagate in great circles linked at an angle with respect to the plane containing the sphere centers.
RESUMEN
We show that homogeneous polymer blend microparticles can be prepared in situ from droplets of dilute solution of codissolved polymers. Provided that the droplet of solution is small enough (<10 mum), solvent evaporation is rapid enough to inhibit phase separation. Thus the polymers that are being mixed need not be miscible, which greatly enhances the applicability of the technique. From analysis of two-dimensional Fraunhofer diffraction (angular scattering) patterns, we show that both the real and the imaginary parts of the refractive index can be tuned by adjustment of the relative weight fractions of polymers in solution.