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At least 55 records · Page 3

Extension of Ostwald Ripening Theory

The objective is to develop models based on the mean field approximation of Ostwald ripening to describe the growth of second phase droplets or crystallites. The models will include time variations in nucleation rate, control of saturation through addition of solute, precipitating agents, changes in temperature, and various surface kinetic effects. Numerical integration schemes have been developed and tested against the asymptotic solution of Liftshitz, Slyozov and Wagner (LSW). A second attractor (in addition to the LSW distribution) has been found and, contrary to the LSW theory, the final distribution is dependent on the initial distribution. A series of microgravity experiments is being planned to test this and other results from this work.

Baird, J.↗

Controlling Vapor Pressure In Hanging-Drop Crystallization

Rate of evaporation adjusted to produce larger crystals. Device helps to control vapor pressure of water and other solvents in vicinity of hanging drop of solution containing dissolved enzyme protein. Well of porous frit (sintered glass) holds solution in proximity to drop of solution containing protein or enzyme. Vapor from solution in frit controls evaporation of solvent from drop to control precipitation of protein or enzyme. With device, rate of nucleation limited to decrease number and increase size (and perhaps quality) of crystals - large crystals of higher quality needed for x-ray diffraction studies of macromolecules.

Carter, Daniel C.↗

Ice-Crystal Fallstreaks from Supercooled Liquid Water Parent Clouds

On 31 December 2001, ice-crystal fallstreaks (e.g., cirrus uncinus, or colloquially "Mare's Tails") from supercooled liquid water parent clouds were observed by ground-based lidars pointed vertically from the Atmospheric Radiation Measurement Southern Great Plains (SGP) facility near Lamont, Oklahoma. The incidence of liquid phase cloud with apparent ice-phase precipitation is investigated. Scenarios for mixed-phase particle nucleation, and fallstreak formation and sustenance are discussed. The observations are unique in the context of the historical reverence given to the commonly observed c h s uncinus fallstreak (wholly ice) versus this seemingly contradictory coincidence of liquid water begetting ice-crystal streaks.

Campbell, James R.↗

Temporal Evolution of the Nanostructure and Phase Compositions in a Model Ni-Al-Cr Alloy

In a Ni-5.2 Al-14.2 Cr at.% alloy with moderate solute supersaturations and a very small gamma/gamma prime lattice parameter misfit, the nanostructural and compositional pathways during gamma prime(L12) precipitation at 873 K are investigated using atom-probe tomography, conventional transmission electron microscopy, and hardness measurements. Nucleation of high number densities (N(sub v) greater than 10(sup 23) per cubic meters) of solute-rich precipitates (mean radius = [R] = 0.75 nm), with a critical nucleus composition of Ni-18.3 plus or minus 0.9 Al-9.3 plus or minus 0.7 Cr at.%, initiates between 0.0833 and 0.167 h. With increasing aging time (a) the solute concentrations decay in spheroidal precipitates ([R] less than 10 nm); (b) the observed early-stage coalescence peaks at maximum N(sub v) in coincidence with the smallest interprecipitate spacing; and (c) the reaction enters a quasi-stationary regime where growth and coarsening operate concomitantly. During this quasi-stationary regime, the c (face-centered cubic)-matrix solute supersaturations decay with a power-law dependence of about -1/3, while the dependencies of [R] and N(sub v) are 0.29 plus or minus 0.05 and -0.64 plus or minus 0.06 at a coarsening rate slower than model predications. Coarsening models allow both equilibrium phase compositions to be determined from the compositional measurements. The observed early-stage coalescence is discussed in further detail.

Sudbrack, Chantal K.↗

A System Concept for the Advanced Post-TRMM Rainfall Profiling Radars

Atmospheric latent heating field is fundamental to all modes of atmospheric circulation and upper mixed layer circulations of the ocean. The key to understanding the atmospheric heating process is understanding how and where precipitation occurs. The principal atmospheric processes which link precipitation to atmospheric circulation include: (1) convective mass fluxes in the form of updrafts and downdrafts; (2) microphysical. nucleation and growth of hydrometeors; and (3) latent heating through dynamical controls on the gravitation-driven vertical mass flux of precipitation. It is well-known that surface and near-surface rainfall are two of the key forcing functions on a number of geophysical parameters at the surface-air interface. Over ocean, rainfall variation contributes to the redistribution of water salinity, sea surface temperature, fresh water supply, and marine biology and eco-system. Over land, rainfall plays a significant role in rainforest ecology and chemistry, land hydrology and surface runoff. Precipitation has also been closely linked to a number of atmospheric anomalies and natural hazards that occur at various time scales, including hurricanes, cyclones, tropical depressions, flash floods, droughts, and most noticeable of all, the El Ninos. From this point of view, the significance of global atmospheric precipitation has gone far beyond the science arena - it has a far-reaching impact on human's socio-economic well-being and sustenance. These and many other science applications require the knowledge of, in a global basis, the vertical rain structures, including vertical motion, rain intensity, differentiation of the precipitating hydrometeors' phase state, and the classification of mesoscale physical structure of the rain systems. The only direct means to obtain such information is the use of a spaceborne profiling radar. It is important to mention that the Tropical Rainfall Measuring Mission (TRMM) have made a great stride forward towards this ultimate goal. The Precipitation Radar (PR) aboard the TRMM satellite is the first ever spaceborne radar dedicated to three-dimensional, global precipitation measurements over the tropics and the subtropics, as well as the detailed synopsis of a wide range of tropical rain storm systems. In only twelve months since launch, the PR, together with other science instruments abroad the satellite have already provided unprecedented insights into the rainfall systems. It is anticipated the a lot more exciting and important rain observations would be made by TRMM throughout its mission duration. While TRMM has provided invaluable data to the user community, it is only the first step towards advancing our knowledge on rain processes and its contributions to climate variability. It is envisioned that a TRMM follow-on mission is needed in such a way to capitalize on the pioneering information provided by TRMM, and its instrument capability must be extended beyond TRMM in such a way to fully address the key science questions from microphysical to climatic time scale. In fact, a number of new and innovative mission concepts have recently put forth for this purpose. Almost all of these new concepts have suggested the utility of a more advanced, high-resolution, Doppler-enabled, vertical profiling radar that can provide multi-parameter observations of precipitation. In this paper, a system concept for a second- gene ration precipitation radar (PR-2) which addresses the above requirements will be described.

Im, Eastwood↗

Evidence of Mineral Dust Altering Cloud Microphysics and Precipitation

Multi-platform and multi-sensor observations are employed to investigate the impact of mineral dust on cloud microphysical and precipitation processes in mesoscale convective systems. It is clearly evident that for a given convection strength,small hydrometeors were more prevalent in the stratiform rain regions with dust than in those regions that were dust free. Evidence of abundant cloud ice particles in the dust sector, particularly at altitudes where heterogeneous nucleation process of mineral dust prevails, further supports the observed changes of precipitation. The consequences of the microphysical effects of the dust aerosols were to shift the precipitation size spectrum from heavy precipitation to light precipitation and ultimately suppressing precipitation.

Min, Qilong↗

A Proposed Pathway for the Nucleation and Crystal Growth of the Tetragonal Form of Lysozyme

A number of factors, the shape and charge distribution anisotropy, multiple components in the solution (buffer + counter ion, precipitant, protein, and water), conformational flexibility, and large numbers of intermolecular contacts, all serve as complicating variables in understanding the nucleation and growth mechanism for macromolecules. Intermolecular contacts include hydrogen bonds, van der Waals, hydrophobic, salt bridges, and ion-mediated contacts. The latter interactions are stronger and give specificity while the others are weaker, more prevalent, and more promiscuous, i.e., can lead to a range of possible molecular interactions. We propose that for tetragonal lysozyme, and by extension many other monomeric proteins, there is a solution-phase assembly process to form 4(sub 3) helix structures that are the basic unit for nucleation. The formation of these structures is continuous and concentration dependent. They subsequently also servc as growth units, with that process then being a recapitulation of the nucleation process. The advantages of solution phase assembly are the immediate burying of the strongest interactions, removing them from subsequent participation in the nucleation and growth process, and the introduction of symmetry into the system, which also assists in the assembly process.

Pusey, Marc L.↗

The Prevalence of Precipitation from Polar Supercooled Clouds

Supercooled clouds substantially impact polar surface energy budgets but large-scale models often underestimate their occurrence, which motivates accurately establishing metrics of basic processes. An analysis of long-term measurements at Utqiaġvik, Alaska, and McMurdo Station, Antarctica, combines lidar-validated use of soundings to identify supercooled cloud layers and colocated ground-based profiling radar measurements to quantify cloud base precipitation. We find that more than 85 % (75 %) of sampled supercooled layers are precipitating over the Arctic (Antarctic) site, with more than 75 % (50 %) precipitating continuously to the surface. Such high frequencies can be reconciled with substantially lesser spaceborne estimates by considering differences in radar hydrometeor detection sensitivity. While ice precipitation into supercooled clouds from aloft is common, we also find that the great majority of supercooled cloud layers without ice falling into them are themselves continuously generating precipitation. Such sustained primary ice formation is consistent with continuous activation of immersion-mode ice nucleating particles (INPs), suggesting that supercooled cloud formation is a principal gateway to ice formation at temperatures greater than ~ −38 °C over polar regions. The prevalence of weak precipitation fluxes is also consistent with supercooled cloud longevity, and with well-observed and widely simulated case studies. An analysis of colocated microwave radiometer retrievals suggests that weak precipitation fluxes can be nonetheless consequential to moisture budgets for supercooled clouds owing to small liquid water paths. Finally, we suggest that these ground-based precipitation rate statistics offer valuable guidance for improving the representation of polar cloud processes in large-scale models.

Polar clouds↗

The Prevalence of Precipitation From Polar Supercooled Clouds

Supercooled clouds substantially impact polar surface energy budgets, but large-scale models often underestimate their occurrence, which motivates accurately establishing metrics of basic processes. An analysis of long-term measurements at Utqiaġvik, Alaska, and McMurdo Station, Antarctica, combines lidar-validated use of soundings to identify supercooled cloud layers and colocated ground-based profiling radar measurements to quantify cloud base precipitation. We find that more than 85 % (75 %) of sampled supercooled layers are precipitating over the Arctic (Antarctic) site, with more than 75 % (50 %) precipitating continuously to the surface. Such high frequencies can be reconciled with substantially lesser spaceborne estimates by considering differences in radar hydrometeor detection sensitivity. While ice precipitation into supercooled clouds from aloft is common, we also find that the great majority of supercooled cloud layers without ice falling into them are themselves continuously generating precipitation. Such sustained primary ice formation is consistent with continuous activation of immersion-mode ice-nucleating particles (INPs), suggesting that supercooled cloud formation is a principal gateway to ice formation at temperatures greater than ∼−38 ∘C over polar regions. The prevalence of weak precipitation fluxes is also consistent with supercooled cloud longevity and with well-observed and widely simulated case studies. An analysis of colocated microwave radiometer retrievals suggests that weak precipitation fluxes can be nonetheless consequential to moisture budgets for supercooled clouds owing to small liquid water paths. The results here also demonstrate that the observed abundance of mixed-phase clouds can vary substantially with instrument sensitivity and methodology. Finally, we suggest that these ground-based precipitation rate statistics offer valuable guidance for improving the representation of polar cloud processes in large-scale models.

Supercooled clouds↗

The Effects of Thermal History on Nucleation of Tetragonal Lysozyme Crystals, or Hot Protein and Cold Nucleation

Chicken egg white lysozyme has a well characterized thermally driven phase transition. Between pH 4.2 and 5.2, the transition temperature, as defined by the point where the tetragonal and orthorhombic solubilities are equal, is a function of the pH, salt (precipitant) type and concentration, and most likely of the buffer concentration as well. This phase transition can be carried out with protein solution alone, prior to addition of precipitant solution. Warming a lysozyme solution above the phase transition point, then cooling it back below this point, has been shown to affect the subsequent nucleation rate, as determined by the numbers and size of crystals formed, but not the growth rate for the tetragonal crystal form . We have now measured the kinetics of this process and investigated its reversibility. The transition effects are progressive with temperature, having a half time of about 1 hour at 37C at pH 4.8. After holding a lysozyme solution at 37C (prior to addition of precipitant) for 16 hours, then cooling it back to 4C no return to the pre-warmed nucleation kinetics are observed after at least 4 weeks. Orthorhombic lysozyme crystals apparently do not undergo the flow-induced growth cessation of tetragonal lysozyme crystals. Putting the protein in the orthorhombic form does not affect the averaged face growth kinetics, only nucleation, for tetragonal crystals. This differential behaviour may be exploited to elucidate how and where flow affects the lysozyme crystal growth process. The presentation will focus on the results of these and ongoing studies in this area.

Burke, Michael↗

TPSAS-NF1676L-10947-DND

There are large uncertainties in quantifying dust effects on the climate because of the limitations on the measurements and observations of dust-cloud-precipitation-dynamics interactions. As a major terrestrial source of atmospheric aerosols, dusts may serve as a significant climate forcing for the changing climate due to its effect on solar and thermal radiation as well as on clouds and precipitation processes. Latest satellites measurements enable us to determine dust loadings and cloud distributions and can potentially be used to reduce the uncertainties in the estimations of aerosol effects on climate. This study uses sensors on various satellites to investigate the impact of mineral dust on cloud microphysical and precipitation processes in convective systems. A trans-Atlantic dust outbreak of Saharan origin occurring in early March 2004 is considered. For the observed convective systems under a given convective strength, small hydrometeors were found more prevalent in the dusty stratiform regions than in those regions that were dust free. Evidence of abundant cloud ice particles in the dust regions, particularly at altitudes where heterogeneous nucleation of mineral dust prevails, further supports the observed changes of clouds and precipitation. These microphysical effects of the dusts on clouds are to shift the size spectrum of precipitation-sized hydrometeors from heavy precipitation to light precipitation and ultimately to suppress precipitation and increase the lifecycle of cloud systems, especially for stratiform clouds.

B Lin↗

Changes in Stratiform Clouds of Mesoscale Convective Complex Introduced by Dust Aerosols

Aerosols influence the earth s climate through direct, indirect, and semi-direct effects. There are large uncertainties in quantifying these effects due to limited measurements and observations of aerosol-cloud-precipitation interactions. As a major terrestrial source of atmospheric aerosols, dusts may serve as a significant climate forcing for the changing climate because of its effect on solar and thermal radiation as well as on clouds and precipitation processes. Latest satellites measurements enable us to determine dust aerosol loadings and cloud distributions and can potentially be used to reduce the uncertainties in the estimations of aerosol effects on climate. This study uses sensors on various satellites to investigate the impact of mineral dust on cloud microphysical and precipitation processes in mesoscale convective complex (MCC). A trans-Atlantic dust outbreak of Saharan origin occurring in early March 2004 is considered. For the observed MCCs under a given convective strength, small hydrometeors were found more prevalent in the dusty stratiform regions than in those regions that were dust free. Evidence of abundant cloud ice particles in the dust regions, particularly at altitudes where heterogeneous nucleation of mineral dust prevails, further supports the observed changes of clouds and precipitation. The consequences of the microphysical effects of the dust aerosols were to shift the size spectrum of precipitation-sized hydrometeors from heavy precipitation to light precipitation and ultimately to suppress precipitation and increase the lifecycle of cloud systems, especially over stratiform areas.

Lin, B.↗

The Growth of Protein Crystals Using McDUCK

Most of the current microgravity crystal growth hardware is optimized to produce crystals within the limited time available on orbit. This often results in the actual nucleation and growth process being rushed or the system not coming to equilibrium within the limited time available. Longer duration hardware exists, but one cannot readily pick out crystals grown early versus those which nucleated and grew more slowly. We have devised a long duration apparatus, the Multi-chamber Dialysis Unit for Crystallization Kinetics, or McDUCK. This apparatus-is a series of protein chambers, stacked upon a precipitant reservoir chamber. All chambers are separated by a dialysis membrane, which serves to pass small molecules while retaining the protein. The volume of the Precipitant chamber is equal to the sum of the volumes of the protein chamber. In operation, the appropriate chambers are filled with precipitant solution or protein solution, and the McDUCK is placed standing upright, with the precipitant chamber on the bottom. The precipitant diffuses upwards over time, with the time to reach equilibration a function of the diffusivity of the precipitant and the overall length of the diffusion pathway. Typical equilibration times are approximately 2-4 months, and one can readily separate rapid from slow nucleation and growth crystals. An advantage on Earth is that the vertical precipitant concentration gradient dominates that of the solute, thus dampening out solute density gradient driven convective flows. However, large Earth-grown crystals have so far tended to be more two dimensional. Preliminary X-ray diffraction analysis of lysozyme crystals grown in McDUCK have indicated that the best, and largest, come from the middle chambers, suggesting that there is an optimal growth rate. Further, the improvements in diffraction resolution have been better signal to noise ratios in the low resolution data, not an increase in resolution overall. Due to the persistently large crystals grown we are currently proposing McDUCK for the growth of macromolecule crystals for use in neutron diffraction studies.

Ewing, Felicia↗

Protein Crystallization

Nucleation, growth and perfection of protein crystals will be overviewed along with crystal mechanical properties. The knowledge is based on experiments using optical and force crystals behave similar to inorganic crystals, though with a difference in orders of magnitude in growing parameters. For example, the low incorporation rate of large biomolecules requires up to 100 times larger supersaturation to grow protein, rather than inorganic crystals. Nucleation is often poorly reproducible, partly because of turbulence accompanying the mixing of precipitant with protein solution. Light scattering reveals fluctuations of molecular cluster size, its growth, surface energies and increased clustering as protein ages. Growth most often occurs layer-by-layer resulting in faceted crystals. New molecular layer on crystal face is terminated by a step where molecular incorporation occurs. Quantitative data on the incorporation rate will be discussed. Rounded crystals with molecularly disordered interfaces will be explained. Defects in crystals compromise the x-ray diffraction resolution crucially needed to find the 3D atomic structure of biomolecules. The defects are immobile so that birth defects stay forever. All lattice defects known for inorganics are revealed in protein crystals. Contribution of molecular conformations to lattice disorder is important, but not studied. This contribution may be enhanced by stress field from other defects. Homologous impurities (e.g., dimers, acetylated molecules) are trapped more willingly by a growing crystal than foreign protein impurities. The trapped impurities induce internal stress eliminated in crystals exceeding a critical size (part of mni for ferritin, lysozyme). Lesser impurities are trapped from stagnant, as compared to the flowing, solution. Freezing may induce much more defects unless quickly amorphysizing intracrystalline water.

Chernov, Alexander A.↗

Microstructural development of protective Al2O3 scales

Microstructural characteristics of Al2O3 scales grown as protective coatings on NiCrAl alloys used in jet engines are described. The alloys were pure or doped with 0.3 percent Zr or Y and oxidized in 1 atm air at 1100 C for 0.1, 1 or 20.0 hr. The scales were then examined under a microscope. Transient epitaxial scales, formed during the 0.1 hr treatment and containing Ni, Cr and Al, consisted of a mosaic of subgrains and precipitates of different phases. The Y and Zr dopants had no effect on the nucleation site locations. The appearance of intergranular porosity at 0.1 hr was exacerbated after the 1 hr treatment. A bimodal void distribution appeared after 20 hr, when no porosity was evident. The detection of local areas of preferred orientation is taken as a spur to further studies of scale growth to gain control of the grain size or even to produce single crystal scales.

Smialek, J. L.↗

Effect of a prior stretch on the aging response of an Al-Cu-Li-Ag-Mg-Zr alloy

Recently, a family of Al-Cu-Li alloys containing minor amounts of Ag, Mg, and Zr and having desirable combinations of strength and toughness were developed. The Weldalite (trademark) alloys exhibit a unique characteristic in that with or without a prior stretch, they obtain significant strength-ductility combinations upon natural and artificial aging. The ultra-high strength (approximately 690 MPa yield strength) in the peak-aged tempers (T6 and T8) were primarily attributed to the extremely fine T(sub 1) (Al2CuLi) or T(sub 1)-type precipitates that occur in these alloys during artificial aging, whereas the significant natural aging response observed is attributed to strengthening from delta prime (Al3Li) and GP zones. In recent work, the aging behavior of an Al-Cu-Li-Ag-Mg alloy without a prior stretch was followed microstructurally from the T4 to the T6 condition. Commercial extrusions, rolled plates, and sheets of Al-Cu-Li alloys are typically subjected to a stretching operation before artificial aging to straighten the extrusions and, more importantly, introduce dislocations to simulate precipitation of strengthening phases such as T(sub 1) by providing relatively low-energy nucleation sites. The goals of this study are to examine the microstructure that evolves during aging of an alloy that was stretch after solution treatment and to compare the observations with those for the unstretched alloy.

Kumar, K. S.↗

Containerless Liquid to Solid Nucleation Pathways in Two Representative Grades of Commercially Available Zirconium

Experimental measurements were conducted to determine the solid metal nucleation pathways of radiatively cooling, molten zirconium spheres of two different commercially available purity grades in a high-vacuum, high-temperature electrostatic levitator. The ensemble distribution of maximum undercooling temperatures was interpreted using Poisson statistics to determine the temperature dependence of the solid metal nucleation rate. For a sample of nominally 99.95% pure zirconium, the results are consistent with heterogeneous solid metal nucleation either on static catalyst particles at least ~30 nm diameter or on a surface coating. For a sample of nominally 99% pure zirconium, however, it appears that heterogeneous solid metal nucleation occurred either on a polydispersion of ~10 nm (mean diameter) static catalyst particles or on dynamic catalyst particles which precipitated from a solution which became supersaturated as the melt cooled. A quantitative analysis of the compositions of both samples suggests that the catalysts probably consisted of one or more of the following elements: niobium, molybdenum, hafnium, and oxygen.

containerless, nucleation, zirconium↗

Ice Nucleation in Deep Convection

The processes controlling production of ice crystals in deep, rapidly ascending convective columns are poorly understood due to the difficulties involved with either modeling or in situ sampling of these violent clouds. A large number of ice crystals are no doubt generated when droplets freeze at about -40 C. However, at higher levels, these crystals are likely depleted due to precipitation and detrainment. As the ice surface area decreases, the relative humidity can increase well above ice saturation, resulting in bursts of ice nucleation. We will present simulations of these processes using a large-eddy simulation model with detailed microphysics. Size bins are included for aerosols, liquid droplets, ice crystals, and mixed-phase (ice/liquid) hydrometers. Microphysical processes simulated include droplet activation, freezing, melting, homogeneous freezing of sulfate aerosols, and heterogeneous ice nucleation. We are focusing on the importance of ice nucleation events in the upper part of the cloud at temperatures below -40 C. We will show that the ultimate evolution of the cloud in this region (and the anvil produced by the convection) is sensitive to these ice nucleation events, and hence to the composition of upper tropospheric aerosols that get entrained into the convective column.

Jensen, Eric↗