Paula Polyak Provencio

Effect of threading dislocations on the Bragg peakwidths of GaN, AlGaN, and AlN heterolayers

We develop a reciprocal-space model that describes the (hkl) dependence of the broadened Bragg peakwidths produced by x-ray diffraction from a dislocated epilayer. We compare the model to experiments and find that it accurately describes the peakwidths of 16 different Bragg reflections in the [010] zone of both GaN and AlN heterolayers. Using lattice-distortion parameters determined by fitting the model to selected reflections, we estimate threading-dislocation densities for seven different GaN and AlGaN samples and find improved agreement with transmission electron microscopy measurements.

Low-dislocation-density GaN from a single growth on a textured substrate

The density of threading dislocations (TD) in GaN grown directly on flat sapphire substrates is typically greater than 10{sup 9}/cm{sup 2}. Such high dislocation densities degrade both the electronic and photonic properties of the material. The density of dislocations can be decreased by orders of magnitude using cantilever epitaxy (CE), which employs prepatterned sapphire substrates to provide reduced-dimension mesa regions for nucleation and etched trenches between them for suspended lateral growth of GaN or AlGaN. The substrate is prepatterned with narrow lines and etched to a depth that permits coalescence of laterally growing III-N nucleated on the mesa surfaces before vertical growth fills the etched trench. Low dislocation densities typical of epitaxial lateral overgrowth (ELO) are obtained in the cantilever regions and the TD density is also reduced up to 1 micrometer from the edge of the support regions.

Misfit dislocation formation in the AlGaN∕GaN heterointerface

Heteroepitaxial growth of AlxGa1−xN alloy films on GaN results in large tensile strain due to the lattice mismatch. During growth, this strain is partially relieved both by crack formation and by the coupled introduction of dense misfit dislocation arrays. Extensive transmission electron microscopy measurements show that the misfit dislocations enter the film by pyramidal glide of half loops on the 1∕3⟨1123⟩∕{1122} slip system, which is a well-known secondary slip system in hcp metals. Unlike the hcp case, however, where shuffle-type dislocations must be invoked for this slip plane, we show that glide-type dislocations are also possible. Comparisons of measured and theoretical critical thicknesses show that fully strained films can be grown into the metastable regime, which we attribute to limitations on defect nucleation. At advanced stages of relaxation, interfacial multiplication of dislocations dominates the strain relaxation process. This work demonstrates that misfit dislocations are important mec...

Optical properties of gold and silver nanoclusters investigated by liquid chromatography

We report high-pressure liquid chromatography (HPLC) and transmission electron microscopy studies of the size-dependent absorbance properties of Au and Ag nanoclusters dispersed in organic solvents. These nanosize metal clusters are synthesized by an inverse micelle synthetic technique at room temperature in inert oils and those investigated range in diameter from 1.3–8 nm. HPLC allows us to separate the clusters from all other chemicals and size select to a resolution of ±2 A. We use an on-line photodiode array to study the size-dependent absorbance properties of these clusters. For both Au and Ag clusters in the size range d=8 to d=1.5 nm, the plasmon linewidth broadens following a 1/R linewidth size dependence whose slope is greatest for Au. The peak asymmetry in the plasmon band shape is greatest for Au and increases with decreasing size for both Au and Ag clusters. The plasmon peak energy blue shifts with decreasing size for Au clusters while in the case of Ag nanoclusters a red shift is observed.We report high-pressure liquid chromatography (HPLC) and transmission electron microscopy studies of the size-dependent absorbance properties of Au and Ag nanoclusters dispersed in organic solvents. These nanosize metal clusters are synthesized by an inverse micelle synthetic technique at room temperature in inert oils and those investigated range in diameter from 1.3–8 nm. HPLC allows us to separate the clusters from all other chemicals and size select to a resolution of ±2 A. We use an on-line photodiode array to study the size-dependent absorbance properties of these clusters. For both Au and Ag clusters in the size range d=8 to d=1.5 nm, the plasmon linewidth broadens following a 1/R linewidth size dependence whose slope is greatest for Au. The peak asymmetry in the plasmon band shape is greatest for Au and increases with decreasing size for both Au and Ag clusters. The plasmon peak energy blue shifts with decreasing size for Au clusters while in the case of Ag nanoclusters a red shift is observed.

Synthesis and Thermoelectric Properties of Bi2Se3 Nanostructures

Bismuth selenide (Bi2Se3) nanostructures were synthesized via solvothermal method. The crystallinity of the as-synthesized sample has been analyzed by X-ray diffraction, which shows the formation of rhombohedral Bi2Se3. Electron microscopy examination indicates that the Bi2Se3 nanoparticles have hexagonal flake-like shape. The effect of the synthesis temperature on the morphology of the Bi2Se3 nanostructures has also been investigated. It is found that the particle size increases with the synthesis temperature. Thermoelectric properties of the Bi2Se3 nanostructures were also measured, and the maximum value of dimensionless figure of merit (ZT) of 0.096 was obtained at 523 K.

Materials modification using intense ion beams

Pulsed intense ion beams have been developed for applications including surface modification and alloying, and thin-film and nanopowder synthesis. Rapid thermal processing with ions is quite promising for large-scale commercial use, due to the high specific ion energy deposition (joules per cubic centimeter) without reflection, and to the relative efficiency and low cost of the pulsed power ion-beam drivers compared to other high-kinetic energy alternatives. We discuss in this paper the basis for the use of ions in materials processing and the methods of beam formation and impingement on material to be treated, and give examples of recent and ongoing work in materials processing.

Highly Versatile Rare Earth Tantalate Pyrochlore Nanophosphors

Rare earth tantalate materials are of considerable interest in energy and environmentally related applications including photocatalytic H(2) generation or contaminant decomposition, ion conductivity for batteries and fuel cells, and phosphors for light-emitting diodes (LEDs). These Eu-doped rare earth tantalate pyrochlore nanoparticles, K(1-2x)LnTa(2)O(7-x):Eu(3+) (Ln = Lu, Y, Gd; x = (1)/(3) for Gd, x = 0 for Lu and Y), have quantum yields up to 78% when excited with blue light (464 nm), which is remarkable for nanoparticle forms that can suffer efficiency loss by surface effects or poor crystallinity, and are furthermore quite suitable for LED applications. The Gd analogue with its framework distortions has particularly high quantum yields. The blue excitation peak matches the emission of the GaN LED. The combination of the high quantum yield under blue excitation, low thermal quenching, and chemical stability renders these new materials promising red phosphors for blue-excitation white LEDs for solid-state lighting. In addition, the pyrochlore lattice is very accommodating to dopants and vacancies and will incorporate virtually any metal and coordination environment ranging from four-coordinate to eight-coordinate. Thus, there are virtually unlimited possibilities for tailoring and optimizing photoluminescent properties, as demonstrated by these scoping studies.

Enhanced thermoelectric figure of merit in SiGe alloy nanowires by boundary and hole-phonon scattering

We report the thermoelectric characteristics of individual p-type SiGe alloy nanowires for diameters of 100 to 300 nm and temperatures between 40 to 300 K. A technique that allows for electrical and thermal characterization on the same nanowire was developed in this work. Experimental data provide evidence of the scattering of low-frequency phonons by the boundary of the nanowires. The thermal conductivities for SiGe alloy nanowires with different free carrier concentrations reveal that the long free path phonons are also scattered by hole-phonon interactions. Combined boundary and hole-phonon scattering mechanisms with alloy scattering resulted in thermal conductivities as low as 1.1 W/m-K at 300 K, which is one of the lowest measured for SiGe alloys and is comparable to that of bulk silica. The enhanced thermal properties observed in this work yielded ZT close to 0.18 at 300 K—more than a factor of 2 higher than the bulk SiGe alloy.

Precise control of multiwall carbon nanotube diameters using thermal chemical vapor deposition

We grow multiwall carbon nanotube (CNT) films using thermal chemical vapor deposition at atmospheric pressure using a mixture of acetylene and nitrogen from a 4-nm-thick Ni film catalyst. CNTs are characterized using electron microscopy and Rutherford backscattering spectrometry. CNTs grown with this method are extremely uniform in diameter, both throughout the sample and within the lengths of individual tubes. Nanotube outer diameters, ranging from 5–350 nm, and the total deposition of carbon material, increase exponentially with growth temperature from 630 °C–790 °C.

Relaxation of compressively strained AlGaN by inclined threading dislocations.

Transmission electron microscopy and x-ray diffraction were used to assess the microstructure and strain of AlxGa1−xN(x=0.61–0.64) layers grown on AlN. The compressively-strained AlGaN is partially relaxed by inclined threading dislocations, similar to observations on Si-doped AlGaN by P. Cantu, F. Wu, P. Waltereit, S. Keller, A. E. Romanov, U. K. Mishra, S. P. DenBaars, and J. S. Speck [Appl. Phys. Lett. 83, 674 (2003)]; however, in our material, the dislocations bend before the introduction of any Si. The bending may be initiated by the greater lattice mismatch or the lower dislocation density of our material, but the presence of Si is not necessarily required. The relaxation by inclined dislocations is quantitatively accounted for with the model of A. E. Romanov and J. S. Speck [Appl. Phys. Lett. 83, 2569 (2003)], and we demonstrate the predicted linear dependence of relaxation on layer thickness. Notably, such relaxation was not found in tensile strained AlGaN grown on GaN [J. A. Floro, D. M. Follstae...