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At least 1,135 records · Page 63

Nucleation, Growth, and Strain Relaxation of Lattice-Mismatched III-V Semiconductor Epitaxial Layers

We have investigated the early stages of evolution of highly strained 2-D InAs layers and 3-D InAs islands grown by metal-organic chemical vapor deposition (MOCVD) on (100) and (111) B GaAs substrates. The InAs epilayer / GaAs substrate combination has been chosen because the lattice-mismatch is severe (approx. 7.20%), yet these materials are otherwise very similar. By examining InAs-on-GaAs composites Instead of the more common In(x)Ga(1-x)As alloy, we remove an additional degree of freedom (x) and thereby simplify data interpretation. A matrix of experiments is described in which the MOCVD growth parameters -- susceptor temperature, TMIn flux, and AsH3 flux -- have been varied over a wide range. Scanning electron microscopy, atomic force microscopy, transmission electron microscopy, and electron microprobe analysis have been employed to observe the thin film surface morphology. In the case of 3-D growth, we have extracted activation energies and power-dependent exponents that characterize the nucleation process. As a consequence, optimized growth conditions have been identified for depositing approx. 250 A thick (100) and (111)B oriented InAs layers with relatively smooth surfaces. Together with preliminary data on the strain relaxation of these layers, the above results on the evolution of thin InAs films indicate that the (111)B orientation is particularly promising for yielding lattice-mismatched films that are fully relaxed with only misfit dislocations at the epilayer / substrate interface.

Welser, R. E.↗

Fluorescence Studies of Protein Crystal Nucleation

We have postulated that, in the case of tetragonal chicken egg white lysozyme, crystal growth occurs by the addition of pre-critical nuclei sized n-mers that form in the bulk solution, and that the n-mer growth units were multiples of the tetrameric 4(sub 3) helical structure. These have the strongest intermolecular bonds in the crystal and are therefore likely to be the first species formed. High resolution AFM studies provide strong supporting evidence for this model, but the data also suggest that the actual species in solution may not be identical in structure to that found in the crystal. We are using fluorescence resonance energy transfer (FRET) to study the initial solution phase self-assembly process, using covalent fluorescent derivatives which crystallize in the characteristic P4(sub 3)2(sub 1)2(sub 1) space group. FRET studies are being carried out between the cascade blue (CB-lys, donor, Ex(sub max) 366 nm, Em 420 nm) and lucifer yellow (LY-lys, acceptor, Ex(sub max) 430 nm, Em 528 nm) asp101 derivatives. The estimated R(sub 0) for this probe pair, the distance where 50% of the donor energy is transferred to the acceptor, is approx. 1.2 nm, compared to 2.2 nm between the side chain carboxyls of adjacent asp101's in the crystalline 4(sub 3) helix. The short donor lifetime of 2.80 ns (chi(sup 2) = 0.644), coupled with the large average distances between the molecules (greater than or equal to 50 nm) in solution, ensure that any energy transfer observed is not due to random diffusive interactions. Lifetime data show that CB-lys has a single lifetime when it is the only species in solution. Similarly, LY-lys also exhibits a single lifetime of 4.63 ns (chi(sup 2) = 0.42) when alone in solution. Addition of LY-lys to CB-lys results in the appearance of a third lifetime component of 0.348ns for the CB-lys. The fractional intensities of the different species present can be used to estimate the distribution of monomer and n-mers in solution. The self-association process is a function of the protein concentration relative to the saturation concentration, and observing it in dilute solution (conc. less than or equal to 10(exp -5)M) requires that the experiments be performed under low solubility conditions, i.e., low temperatures and high salt concentrations. Data from preliminary steady state FRET studies with N-terminal bound pyrene acetic acid (PAA-lys, donor, Ex 340 nm, Em 376 nm) and asp101 LY-lys as an acceptor showed a consistent trend of decreasing donor fluorescence intensity with increasing total protein concentration. The FRET data have been obtained at pH 4.6, 0.1M NaAc buffer, at 5 and 7% NaCl, 4 C. The corresponding C(sub sat) values are 0.471 and 0.362 mg/ml (approx. 3.3 and approx. 2.5 x 10(exp -5)M respectively). The donor fluorescence decrease is more pronounced at7% NaCl, consistent with the expected increased intermolecular interactions at higher salt concentrations as reflected in the lower solubility. Results from these and other ongoing studies will be discussed in conjunction with an emerging model for how tetragonal lysozyme crystals nucleate and the relevance of that model to other proteins.

Pusey, Marc↗

Quantifying Main Trends in Lysozyme Nucleation: The Effects of Precipitant Concentration, Supersaturation and Impurities

Full factorial experimental design incorporating multi-linear regression analysis of the experimental data allows quick identification of main trends and effects using a limited number of experiments. In this study these techniques were employed to identify the effect of precipitant concentration, supersaturation, and the presence of an impurity, the physiological lysozyme dimer, on the nucleation rate and crystal dimensions of the tetragonal forin of chicken egg white lysozyme. Decreasing precipitant concentration, increasing supers aturation, and increasing impurity, were found to increase crystal numbers. The crystal axial ratio decreased with increasing precipitant concentration, independent of impurity.

Burke, Michael W.↗

Kinetics of Nucleation and Crystal Growth in Glass Forming Melts in Microgravity

This flight definition project has the specific objective of investigating the kinetics of nucleation and crystal growth in high temperature inorganic oxide, glass forming melts in microgravity. It is related to one of our previous NASA projects that was concerned with glass formation for high temperature containerless melts in microgravity. The previous work culminated in two experiments which were conducted aboard the space shuttle in 1983 and 1985 and which consisted of melting (at 1500 C) and cooling levitated 6 to 8 mm diameter spherical samples in a Single Axis Acoustic Levitator (SAAL) furnace. Compared to other types of materials, there have been relatively few experiments, 6 to 8, conducted on inorganic glasses in space. These experiments have been concerned with mass transport (alkali diffusion), containerless melting, critical cooling rate for glass formation, chemical homogeneity, fiber pulling, and crystallization of glass forming melts. One of the most important and consistent findings in all of these experiments has been that the glasses prepared in microgravity are more resistant to crystallization (better glass former) and more chemically homogeneous than equivalent glasses made on Earth (1 g). The chemical composition of the melt appears relatively unimportant since the same general results have been reported for oxide, fluoride and chalcogenide melts. These results for space-processed glasses have important implications, since glasses with a higher resistance to crystallization or higher chemical homogeneity than those attainable on Earth can significantly advance applications in areas such as fiber optics communications, high power laser glasses, and other photonic devices where glasses are the key functional materials.

Day, Delbert E.↗

Studies of Ice Nucleating Aerosol Particles in Arctic Cloud Systems

The focus of this research is to improve the understanding of ice nucleating aerosol particles (IN) and the role they play in ice formation in Arctic clouds. IN are important for global climate issues in a variety of ways. The primary effect is their role in determining the phase (liquid or solid) of cloud particles. The microscale impact is on cloud particle size, growth rate, shape, fall speed, concentration, radiative properties, and scavenging of gases and aerosols. On a larger scale, ice formation affects the development of precipitation (rate, amount, type, and distribution), latent heat release (rate and altitude), ambient humidity, the persistence of clouds, and cloud albedo. The overall goals of our FIRE 3 research are to characterize the concentrations and variability of Arctic IN during the winter-spring transition, to compare IN measurements with ice concentrations in Arctic clouds, and to examine selected IN samples for particle morphology and chemical there are distinguishable chemical signatures. The results can be combined with other measurements of aerosols, gaseous species, and cloud characteristics in order to understand the processes that determine the phase and concentration of cloud particles.

Rogers, David C.↗

Evolution of Vapor Bubbles Nucleation Sites in Low Gravity

When liquid is expelled by a vapor bubble growing at a nucleation site on a superheated surface, a thin microlayer underneath the bubble is left behind. It is evaporated from the free microlayer surface that provides for bubble growth. The average thickness of the microlayer determining the evaporation rate increases with time if the latter does not exceed a threshold value associated with the burn-out crisis. The bubble is described as a spherical segment with its flattened part adjoining the microlayer. This introduces two independent variables - the radius of the spherical part of the bubble surface and the polar angle that defines the relative area of the flattened part. They are to be found out from a set of two strongly nonlinear equations resulting from mass and momentum conservation laws. The first one depends on both microlayer thickness and nonmonotonously changing bubble base area. The second involves two major factors favoring bubble detachment - the buoyancy and a force due to the initial momentum of vapor input into the bubble. The former force depends on gravity whereas the latter one does not. It is why the limiting regimes of bubble evolution that correspond to normal or moderately reduced gravity and to microgravity feature drastically different properties. In the first case, the buoyancy dominates and the bubble evolves in such a manner as to become a full sphere at a moment that can be viewed as that of detachment. The detachment volume grows as gravity decreases. In the second case, the buoyancy is negligible and the bubble stays near the surface, while its volume continues to increase for a sufficiently long time. The findings are discussed in connection with experimental data obtained under different gravity conditions, some unpublished experiments being included. They help to understand why the pool boiling heat transfer coefficient frequently increases as gravity falls down and eventually vanishes.

Buyevich, Yu A.↗

Modeling of Vapor Bubble Growth Under Nucleate Boiling Conditions in Reduced Gravity

A dynamic model is developed to describe the evolution of a vapor bubble growing at a nucleation site on a superheated surface under arbitrary gravity. The bubble is separated from the surface by a thin microlayer and grows due to the evaporation from the microlayer interface. The average thickness of the microlayer increases as the bubble expands along the surface if the evaporation rate is lower than some critical value. The corresponding threshold value of the surface temperature has to be associated with the burn-out crisis. Two main reasons make for bubble separation, which are the buoyancy force and a force caused by the vapor momentum that comes to the bubble with vapor molecules. The latter force is somewhat diminished if condensation takes place at the upper bubble surface in subcooled liquids. The action of the said forces is opposed by inertia of the additional mass of liquid as the bubble center rises above the surface and by inertia of liquid being expelled by the growing bubble in radial directions. An extra pressure force arises due to the liquid inflow into the microlayer with a finite velocity. The last force helps in holding the bubble close to the surface during an initial stage of bubble evolution. Two limiting regimes with distinctly different properties can be singled out, depending on which of the forces that favor bubble detachment dominates. Under conditions of moderately reduced gravity, the situation is much the same as in normal gravity, although the bubble detachment volume increases as gravity diminishes. In microgravity, the buoyancy force is negligible. Then the bubble is capable of staying near the surface for a long time, with intensive evaporation from the microlayer. It suggests a drastic change in the physical mechanism of heat removal as gravity falls below a certain sufficiently low level. Inferences of the model and conclusions pertaining to effects caused on heat transfer processes by changes in bubble hydrodynamics induced by gravity are discussed in connection with experimental evidence, both available in current and in as yet unpublished literature.

Buyevich, Yu A.↗

Nucleation of Quantized Vortices from Rotating Superfluid Drops

The long-term goal of this project is to study the nucleation of quantized vortices in helium II by investigating the behavior of rotating droplets of helium II in a reduced gravity environment. The objective of this ground-based research grant was to develop new experimental techniques to aid in accomplishing that goal. The development of an electrostatic levitator for superfluid helium, described below, and the successful suspension of charged superfluid drops in modest electric fields was the primary focus of this work. Other key technologies of general low temperature use were developed and are also discussed.

Donnelly, Russell J.↗

Ice Nucleation Processes in Upper Tropospheric Wave-Clouds Observed During SUCCESS

We have compared in situ measurements near the leading-edges of wave-clouds observed during the SUCCESS experiment with numerical modeling of ice nucleation. Observations of high supersaturations with respect to ice (\geq 150\%) near the leading edge of a very cold wave cloud (T < --60^\circC) are consistent with recent theoretical and laboratory studies suggesting that large supersaturations are required to homogeneously freeze sulfate aerosols. Also, the peak ice crystal number densities observed in this cloud (about 4cm -3/sup>) are consistent with the number densities calculated in our model. The consistency between model results (using homogeneous freezing and the observations indicates that the number density of effective heterogeneous ice nuclei must be no more than about 2 cm -3 . In the warmer wave-cloud (T (approx.)eq --37^\circC) relatively large ice number densities were observed (20--40 cm -3 . Our model calculations suggest that these large number densities are only possible if liquid droplets were activated at the cloud leading-edge, followed by subsequent homogeneous freezing. If sulfate aerosols had frozen before liquid droplets could be activated, then the peak ice crystal number density should have been less than 10 cm -3 .

Jensen, E. J.↗

Studies of Nucleation and Growth, Specific Heat and Viscosity of Undercooled Melts of Quasicrystals and Polytetrahedral-Phase-Forming Alloys

The local atomic structures of undercooled liquid metals are presumed to be icosahedral; this order is incompatible with translational periodicity, constituting a barrier to the nucleation of the crystal phase. The extended atomic structure of the icosahedral quasicrystal (i-phase) is similar to that presumed in the undercooled liquid. Therefore, a comparison of the maximum undercooling in alloys that form the i-phase with those that form crystal phases provides a probe of the liquid structure.

Kelton, K. F.↗

The Connection Between Local Icosahedral Order in Metallic Liquids and the Nucleation of Ordered Phases

Over fifty years ago, David Turnbull showed that the temperature of many metallic liquids could be decreased far below their equilibrium melting temperature before crystallization occurred. To explain those surprising results, Charles Frank hypothesized that the local structures of undercooled metallic liquids are different from those of crystal phases, containing a significant degree of icosahedral order that is incompatible with extended periodicity. Such structural differences must create a barrier to the formation crystal phases, explaining the observed undercooling behavior. If true, the nucleation from the liquid of phases with extended icosahedral order should be easier. Icosahedral order is often favored in small clusters, as observed recently in liquid-like clusters of pure Pb on the (111) surface of Si(3), for example. However, it has never been shown that an increasing preference for icosahedral phase formation can be directly linked with the development of icosahedral order in the undercooled liquid. Owing to the combination of very recent advances in levitation techniques and the availability of synchrotron X-ray and high flux neutron facilities.

Kelton, K. F.↗

Tetragonal Lysozyme Nucleation and Crystal Growth: The Role of the Solution Phase

Experimental evidence indicates a dominant role of solution phase interactions in nucleating and growing tetragonal lysozyme crystals. These interactions are extensive, even at saturation, and may be a primary cause of misoriented regions in crystals grown on Earth. Microgravity, by limiting interfacial concentrations to diffusion-controlled levels, may benefit crystal quality by also reducing the extent of associated species present at the interface.

Pusey, Marc L.↗

The Connection Between Local Icosahedral Order in Metallic Liquids and the Nucleation of Ordered Phases

Over fifty years ago, David Turnbull showed that the temperature of many metallic liquids could be decreased far below their equilibrium melting temperature before crystallization occurred. To explain those surprising results, Charles Frank hypothesized that the local structures of undercooled metallic liquids are different from those of crystal phases, containing a significant degree of icosahedral order that is incompatible with extended periodicity. Such structural differences must create a barrier to the formation crystal phases, explaining the observed undercooling behavior. If true, the nucleation from the liquid of phases with extended icosahedral order should be easier. Icosahedral order is often favored in small clusters, as observed recently in liquid-like clusters of pure Pb on the (111) surface of Si, for example. However, it has never been shown that an increasing preference for icosahedral phase formation can be directly linked with the development of icosahedral order in the undercooled liquid. Owing to the combination of very recent advances in levitation techniques and the availability of synchrotron x-ray and high flux neutron facilities, this is shown here.

Curreri, Peter A.↗

The Connection Between Local Icosahedral Order in Metallic Liquids and the Nucleation Behavior of Ordered Phases

Over fifty years ago, David Turnbull showed that the temperature of many metallic liquids could be decreased far below their equilibrium melting temperature before crystallization occurred. To explain those surprising results, Charles Frank hypothesized that the local structures of undercooled metallic liquids are different from those of crystal phases, containing a significant degree of icosahedral order that is incompatible with extended periodicity. Such structural differences must create a barrier to the formation crystal phases, explaining the observed undercooling behavior. If true, the nucleation from the liquid of phases with extended icosahedral order should be easier. Icosahedral order is often favored in small clusters, as observed recently in liquid-like clusters of pure Pb on the (111) surface of Si[3], for example. However, it has never been shown that an increasing preference for icosahedral phase formation can be directly linked with the development of icosahedral order in the undercooled liquid. Owing to the combination of very recent advances in levitation techniques and the availability of synchrotron x-ray and high flux neutron facilities, this is shown here.

Kelton, K. F.↗

Transport Phenomena in Thin Rotating Liquid Films Including: Nucleate Boiling

In this grant, experimental, numerical and analytical studies of heat transfer in a thin liquid film flowing over a rotating disk have been conducted. Heat transfer coefficients were measured experimentally in a rotating disk heat transfer apparatus where the disk was heated from below with electrical resistance heaters. The heat transfer measurements were supplemented by experimental characterization of the liquid film thickness using a novel laser based technique. The heat transfer measurements show that the disk rotation plays an important role on enhancement of heat transfer primarily through the thinning of the liquid film. Experiments covered both momentum and rotation dominated regimes of the flow and heat transfer in this apparatus. Heat transfer measurements have been extended to include evaporation and nucleate boiling and these experiments are continuing in our laboratory. Empirical correlations have also been developed to provide useful information for design of compact high efficiency heat transfer devices. The experimental work has been supplemented by numerical and analytical analyses of the same problem. Both numerical and analytical results have been found to agree reasonably well with the experimental results on liquid film thickness and heat transfer Coefficients/Nusselt numbers. The numerical simulations include the free surface liquid film flow and heat transfer under disk rotation including the conjugate effects. The analytical analysis utilizes an integral boundary layer approach from which

Faghri, Amir↗

Modeling Nucleation and Grain Growth in the Solar Nebula: Initial Progress Report

The primitive solar nebula was a violent and chaotic environment where high energy collisions, lightning, shocks and magnetic re-connection events rapidly vaporized some fraction of nebular dust, melted larger particles while leaving the largest grains virtually undisturbed. At the same time, some tiny grains containing very easily disturbed noble gas signatures (e.g., small, pre-solar graphite or SiC particles) never experienced this violence, yet can be found directly adjacent to much larger meteoritic components (chondrules or CAIs) that did. Additional components in the matrix of the most primitive carbonaceous chondrites and in some chondritic porous interplanetary dust particles include tiny nebular condensates, aggregates of condensates and partially annealed aggregates. Grains formed in violent transient events in the solar nebula did not come to equilibrium with their surroundings. To understand the formation and textures of these materials as well as their nebular abundances we must rely on Nucleation Theory and kinetic models of grain growth, coagulation and annealing. Such models have been very uncertain in the past: we will discuss the steps we are taking to increase their reliability.

Nuth, Joseph A.↗

Complex fracture nucleation and evolution with nonlocal elastodynamics

In this study, a mechanical model is introduced for predicting the initiation and evolution of complex fracture patterns without the need for damage variable or law. The model, a continuum variant of Newton's second law, uses integral rather than partial differential operators where the region of integration is over finite domain. The force interaction is derived from a novel nonconvex strain energy density function, resulting in a nonmonotomic material model. The resulting equation of motion is proved to be mathematically well-posed. The model has the capacity to simulate nucleation and growth of multiple, mutually interacting dynamic fractures. In the limit of zero region of integration, the model reproduces the classic Griffith model of brittle fracture. The simplicity of the formulation avoids the need for supplemental kinetic relations that dictate crack growth or the need for an explicit damage evolution law.

36 MATERIALS SCIENCE↗