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Airborne particulate matter and spacecraft internal environments
Instrumentation, consisting of a Shuttle Particle Sampler (SPS) and a Shuttle Particle Monitor (SPM), has been developed to characterize the airborne particulate matter in the Space Shuttle cabin during orbital flight. The SPS size selectively collects particles in four size fractions (0-2.5, 2.5-10, 10-100, and greater than 100 microns) which are analyzed postflight for mass concentration and size distribution, elemental composition, and morphology. The SPM provides a continuous record of particle concentration through photometric light scattering. Measurements were performed onboard Columbia, OV-102, during the flight of STS-32 in January 1990. No significant changes were observed in the particle mass concentration, size distribution, or chemical composition in samples collected during flight-day 2 and flight-day 7. The total mass concentration was 56 microg/cu cm with approximately half of the particles larger than 100 microns. Elemental analysis showed that roughly 70 percent of the particles larger than 2.5 microns were carbonaceous with small amounts of other elements present. The SPM showed no temporal or spatial variation in particle mass concentration during the mission.
A Tracking Sun Photometer Without Moving Parts
This innovation is small, lightweight, and consumes very little electricity as it measures the solar energy attenuated by gases and aerosol particles in the atmosphere. A Sun photometer is commonly used on the Earth's surface, as well as on aircraft, to determine the solar energy attenuated by aerosol particles in the atmosphere and their distribution of sizes. This information is used to determine the spatial and temporal distribution of gases and aerosols in the atmosphere, as well as their distribution sizes. The design for this Sun photometer uses a combination of unique optics and a charge coupled device (CCD) array to eliminate moving parts and make the instrument more reliable. It could be selfcalibrating throughout the year. Data products would be down-welling flux, the direct-diffuse flux ratio, column abundance of gas phase constituents, aerosol optical depth at multiple-wavelengths, phase functions, cloud statistics, and an estimate of the representative size of atmospheric particles. These measurements can be used to obtain an estimate of aerosol size distribution, refractive index, and particle shape. Incident light is received at a light-reflecting (inner) surface, which is a truncated paraboloid. Light arriving from a hemispheric field of view (solid angle 2 steradians) enters the reflecting optic at an entrance aperture at, or adjacent to, the focus of the paraboloid, and is captured by the optic. Most of this light is reflected from an inner surface. The light proceeds substantially parallel to the paraboloid axis, and is detected by an array detector located near an exit aperture. Each of the entrance and exit apertures is formed by the intersection of the paraboloid with a plane substantially perpendicular to the paraboloid axis. Incident (non-reflected) light from a source of limited extent (the Sun) illuminates a limited area on the detector array. Both direct and diffuse illumination may be reflected, or not reflected, before being received on the detector array. As the Sun traverses a path in the sky over some time interval, the track of the Sun can be traced on the detector array. A suitably modified Sun photometer might be used to study the dynamics of an environment on another planet or satellite with an atmosphere.
Aerosol-Cloud Interactions during Tropical Deep Convection: Evidence for the Importance of Free Tropospheric Aerosols
NASA's 2002 CRYSTAL-FACE field experiment focused on the formation and evolution of tropical cirrus cloud systems in southern Florida. Multiple aircraft extensively sampled cumulonimbus dynamical and microphysical properties, as well as characterizing ambient aerosol populations both inside and outside the full depth of the convective column. On July 18, unique measurements were taken when a powerful updraft was traversed directly by aircraft, providing a window into the primary source region of cumulonimbus anvil crystals. Observations of the updraft, entered at approximately l0 km altitude and -34 C, indicated more than 200 cloud particles per mL at vertical velocities exceeding 20 m/s and the presence of significant condensation nuclei and liquid water within the core. In this work, aerosol and cloud phase observations are integrated by simulating the updraft conditions using a large-eddy resolving model with 3 explicit multiphase microphysics, including treatment of size-resolved aerosol fields, aerosol activation and freezing, and evaporation of cloud particles back to the aerosol phase. Simulations were initialized with observed thermodynamic and aerosol size distributions profiles and convection was driven by surface fluxes assimilated from the ARPS forecast model. Model results are consistent with the conclusions that most crystals are homogeneously frozen droplets and that entrained free tropospheric aerosols may contribute a significant fraction of the crystals. Thus most anvil crystals appear to be formed aloft in updraft cores, well above cloud base. These conclusions are supported by observations of hydrometeor size distribution made while traversing the dore, as well as aerosol and cloud particle size distributions generally observed by aircraft below 4km and crystal properties generally observed by aircraft above 12km.
Viking Lander image analysis of Martian atmospheric dust
We have reanalyzed three sets of Viking Lander 1 and 2 (VL1 and VL2) images of the Martian atmosphere to better evaluate the radiative properties of the atmospheric dust particles. The properties of interest are the first two moments of the size distribution, the single-scattering albedo, the dust single-scattering phase function, and the imaginary index of refraction. These properties provide a good definition of the influence that the atmospheric dust has on heating of the atmosphere. Our analysis represents a significant improvement over past analyses (Pollack et al. 1977, 1979) by deriving more accurate brightness closer to the sun, by carrying out more precise analyses of the data to acquire the quantities of interest, and by using a better representation of scattering by nonspherical particles. The improvements allow us to better define the diffraction peak and hence the size distribution of the particles. For a lognormal particle size distribution, the first two moments of the size distribution, weighted by the geometric cross section, are found. The geometric cross-section weighted mean radius r(sub eff) is found to be 1.85 +/- 0.3 micrometers at VL2 during northern summer when dust loading was low and 1.52 +/- 0.3 micrometers at VL1 during the first dust storm. In both cases the best cross-section weighted mean variance nu(sub eff) of the size distribution is equal to 0.5 +/- 0.2 micrometers. The changes in size distribution, and thus radiative properties, do not represent a substantial change in solar energy deposition in the atmosphere over the Pollak et al. (1977, 1979) estimates.
Viking Lander image analysis of Martian atmospheric dust
We have reanalyzed three sets of Viking Lander 1 and 2 (VL1 and VL2) images of the Martian atmosphere to better evaluate the radiative properties of the atmospheric dust particles. The properties of interest are the first two moments of the size distribution, the single-scattering albedo, the dust single-scattering phase function, and the imaginary index of refraction. These properties provide a good definition of the influence that the atmospheric dust has on heating of the atmosphere. Our analysis represents a significant improvement over past analyses (Pollack et al. 1977,1979) by deriving more accurate brightnesses closer to the sun, by carrying out more precise analyses of the data to acquire the quantities of interest, and by using a better representation of scattering by nonspherical particles. The improvements allow us to better define the diffraction peak and hence the size distribution of the particles. For a lognormal particle size distribution, the first two moments of the size distribution, weighted by the geometric cross section, are found. The geometric cross-section weighted mean radius (r(sub eff)) is found to be 1.85 +/- 0.3 microns at VL2 during northern summer when dust loading was low and 1.52 +/- 0.3 microns at VL1 during the first dust storm. In both cases the best cross-section weighted mean variance (nu(eff)) of the size distribution is equal to 0.5 +/- 0.2 microns. The changes in size distribution, and thus radiative properties, do not represent a substantial change in solar energy deposition in the atmosphere over the Pollack et al. (1977,1979) estimates.
A test of the applicability of independent scattering to high albedo planetary regoliths
We show that 'independent scattering' is a useful approximation for high albedo particles whose size and packing density are similar to typical particles in the lunar regolith. Laboratory measurements of the intensity and linear polarization of light scattered from a laboratory sample of glass spheres of know size and composition are compared to radiative transfer calculations of the same observable quantities. Mie scattering is integrated over the size distribution of the particles to determine the mean phase and polarization functions, or phase matrix, of the particle. Assuming that the particles scatter independently, the 'doubling method' is used to rigorously calculate multiple scattering in an optically thick layer of these anisotropically scattering particles. All of the major features 'predicted' in the calculated intensity (double peaks at small phase angles) and polarization (negative branch at small phase angles, large positive peak near 20 degrees phase, and small polarization elsewhere) are observed in the laboratory measurements, with good quantitative agreement indicated at phase angles less than 90 degrees. Even though the particles are supported by physical contact with each other in the sample, as are the particles in planetary regoliths, the independent scattering calculation yields a good approximation to both the intensity and polarization. The physical parameters input to the calculation are only the size distribution of the particles and their complex index of refraction (composition). Significant advantages of this approach are that the phase matrix is calculated from basic physical principles and both the intensity and polarization are determined simultaneously. This model may have broad applications to the interpretation of photometry, spectroscopy, and polarimetry of the icy regoliths of high albedo satellites. The intent of this effort is to perform a controlled experiment that tests the utility of the independent scattering assumption
Fundamental Studies of the Reforming of Oxygenated Compounds over Supported Metal Catalysts
The main objective of our research has been to elucidate fundamental concepts associated with controlling the activity, selectivity, and stability of bifunctional, metal-based heterogeneous catalysts for tandem reactions, such as liquid-phase conversion of oxygenated hydrocarbons derived from biomass. We have shown that bimetallic catalysts that combine a highly-reducible metal (e.g., platinum) with an oxygen-containing metal promoter (e.g., molybdenum) are promising materials for conversion of oxygenated hydrocarbons because of their high activity for selective cleavage for carbon-oxygen bonds. We have developed methods to stabilize metal nanoparticles against leaching and sintering under liquid-phase reaction conditions by using atomic layer deposition (ALD) to apply oxide overcoat layers. We have used controlled surface reactions to produce bimetallic catalysts with controlled particle size and controlled composition, with an important application being the selective conversion of biomass-derived molecules. The synthesis of catalysts by traditional methods may produce a wide distribution of metal particle sizes and compositions; and thus, results from spectroscopic and reactions kinetics measurements have contributions from a distribution of active sites, making it difficult to assess how the size and composition of the metal particles affect the nature of the surface, the active sites, and the catalytic behavior. Thus, we have developed methods to synthesize bimetallic nanoparticles with controlled particle size and controlled composition to achieve an effective link between characterization and reactivity, and between theory and experiment. We have also used ALD to modify supported metal catalysts by addition of promoters with atomic-level precision, to produce new bifunctional sites for selective catalytic transformations. We have used a variety of techniques to characterize the metal nanoparticles in our catalysts, including scanning transmission electron microcopy (STEM) to measure size and structure, energy dispersive X-ray spectroscopy (EDS) to measure atomic composition, X-ray absorption spectroscopy (XAS) to measure oxidation state and metal coordination, Fourier transform infrared spectroscopy (FTIR) to study adsorbed species, laser Raman spectroscopy to probe metal oxide promoters, and temperature programmed reaction/desorption to study the energetics of adsorption and desorption processes. We have studied our bimetallic catalysts for the selective cleavage of carbon-oxygen bonds, and we have studied the effects of adding metal oxide promoters to supported platinum and gold catalysts for water-gas shift (i.e., the production of hydrogen by reaction of carbon monoxide with water). We anticipate that the knowledge obtained from our studies will allow us to identify promising directions for new catalysts that show high activity, selectivity, and stability for important reactions, such as the conversion of biomass-derived oxygenated hydrocarbons to fuels and chemicals.
Resolving Detonation NanoDiamond Size Evolution and Morphology at Sub-Microsecond Time-Scales During High-Explosive Detonations
Characterization of the initial morphology of detonation nanodiamond (DND) has been the focus of many research studies that aim to develop fundamental understanding of carbon condensation under extreme conditions. Identifying the pathways of DND formation has the potential for significant impact in many of the controlled synthesis of nanoscale carbon with tailored functionality; currently, a wide range of possible (and conflicting) mechanisms of nucleation and growth have been proposed and further research is essential. Building a comprehensive understanding of DND formation is challenging because it requires in situ characterization on the sub-µs time-scale during a high explosive detonation. In this study, time resolved small angle X-ray scattering (TR-SAXS) is used to reveal the early-stage DND morphology from < 0.1 μs to 6 μs after the detonation front passes through the X-ray beam path. We address the ambiguity of models previously reported for analysis of small angle scattering from DND by comparing (i) in situ, TR-SAXS recorded during early-stage particulate formation and (ii) ex situ SAXS and transmission electron microscopy measurements (TEM) of products recovered from detonation of the same high-explosive within a carefully designed ice chamber. The SAXS from both late-time ( > 1 μs) in situ and recovered DND exhibit consistent features in the I(q) curve. Such close similarity allows a high fidelity SAXS model derived from the ex situ SAXS and TEM measurements to be applied to the in situ data, which yields new insight into the early stage (< 1µs) morphology of DND. Our analysis indicates a size-distribution of DND particles is observed within 0.1 μs post-detonation and have a mean core diameter slightly below 4 nm and surface texture that consists of hemispherical protrusions that extend ~ 1 nm from the surface. Beyond ~ 0.3 μs, the size distribution increases slightly, while the surface texture persists for several microseconds after the detonation. Combined with thermochemical simulations, these results indicate that during detonation of Composition B, carbon is condensed into nanoscale diamond much faster than previously reported in other studies. Furthermore, the surface texture of the DND is shown to arise during condensation rather than via subsequent graphitization.
Ice nucleation activity of rocket effluent
An investigation was conducted concerning the ice nucleation activity of the exhaust products of solid rockets. The Voyager I and II payloads were launched from Kennedy Space Center on September 5 and August 20, 1977, respectively. A visible stabilized ground cloud (SGC) consisting of rocket effluent and dust formed downwind. An instrumented aircraft was used to make multiple passes in the SGC. A Mylar bag was rapidly filled with SGC aerosol and then immediately sampled with an ice nucleus counter. Analyses of rocket effluent collected are discussed, taking into account the ice nucleus concentration, particle concentration and size distribution, and the elemental composition of individual particles. A description of laboratory experiments is also presented, giving attention to the elemental composition of individual particles and the ice nucleus concentration.
Seeded Growth of Colloidal Silica Particles
The method of seeded growth was studied for producing mondisperse colloidal silica particles. It was shown that particle size as well as weight percent solids could be controlled by using this method. The particles were characterized by transmission electron microscopy (TEM) and quasielastic light scattering (QELS). The particles were found to have a bimodal size distribution when examined by TEM. The particle size as determined by QELS was found to be roughly 10-20% larger than the particle size as determined by TEM. Furthermore, the polydispersity (standard deviation/mean particle size) as determined by QELS was found to be significantly lower than the polydispersity as determined by TEM. This underscores the importance of using TEM as a characterization technique for determining particle monodispersity. It was also noted that there was an increase in particle roughness as the weight percent of the silica particles increased and a new nucleation of particles was observed as the weight percent approached 13%. A recipe for producing monodisperse silica particles in the 150 nm size range is presented.
Multiscale characterization and comparison of historical and modern nuclear graphite grades
Beginning with Chicago Pile I, graphite has been used as a moderator material in nuclear power stations and is considered a potential material for use in future Generation IV advanced reactors. The microstructure of graphite is responsible for much of its mechanical and thermo-physical properties, and how it responds to irradiation. To understand graphite microstructure, it is necessary to understand its porosity at the macro- and micro-scales; and to understand its porosity, it is necessary to characterize the morphological connectivity of the void content and the two main phases of graphite: filler and binder. Here, using several microscopy and analytical techniques, a detailed examination of the heterogeneity, microstructure and pore structure of different graphite grades and their binder and filler phases is presented. Significant differences were found between coarser and finer nuclear grades. Coarse grades have a more diverse range of filler particles, pores and thermal cracks. Finer grades have a more well-defined pore size distribution, fewer variations of filler particles sizes and do not contain as many large thermal cracks. Fine grades tend to have a well-connected network of pores whereas coarser grades contain a larger content of closed porosity. The framework developed within this work can be applied and used to assess the various graphite grades that would down-select materials for specific use in graphite moderated reactor designs.
Geometrical characterization of perlite-metal syntactic foam
This paper introduces an improved method for the detailed geometrical characterization of perlite-metal syntactic foam. This novel metallic foam is created by infiltrating a packed bed of expanded perlite particles with liquid aluminium alloy. The geometry of the solidified metal is thus defined by the perlite particle shape, size and morphology. The method is based on a segmented micro-computed tomography data and allows for automated determination of the distributions of pore size, sphericity, orientation and location. The pore (i.e. particle) size distribution and pore orientation is determined by a multi-criteria k-nearest neighbour algorithm for pore identification. The results indicate a weak density gradient parallel to the casting direction and a slight preference of particle orientation perpendicular to the casting direction. - Highlights: •A new method for identification of pores in porous materials was developed. •It was applied on perlite-metal syntactic foam samples. •A porosity decrease in the axial direction of the samples was determined. •Pore shape analysis showed a high percentage of spherical pores. •Orientation analysis showed that more pores are oriented in the radial direction.
A New Look into the Effect of Large Drops on Radiative Transfer Process
Recent studies indicate that a cloudy atmosphere absorbs more solar radiation than any current 1D or 3D radiation model can predict. The excess absorption is not large, perhaps 10-15 W/sq m or less, but any such systematic bias is of concern since radiative transfer models are assumed to be sufficiently accurate for remote sensing applications and climate modeling. The most natural explanation would be that models do not capture real 3D cloud structure and, as a consequence, their photon path lengths are too short. However, extensive calculations, using increasingly realistic 3D cloud structures, failed to produce photon paths long enough to explain the excess absorption. Other possible explanations have also been unsuccessful so, at this point, conventional models seem to offer no solution to this puzzle. The weakest link in conventional models is the way a size distribution of cloud particles is mathematically handled. Basically, real particles are replaced with a single average particle. This "ensemble assumption" assumes that all particle sizes are well represented in any given elementary volume. But the concentration of larger particles can be so low that this assumption is significantly violated. We show how a different mathematical route, using the concept of a cumulative distribution, avoids the ensemble assumption. The cumulative distribution has jumps, or steps, corresponding to the rarer sizes. These jumps result in an additional term, a kind of Green's function, in the solution of the radiative transfer equation. Solving the cloud radiative transfer equation with the measured particle distributions, described in a cumulative rather than an ensemble fashion, may lead to increased cloud absorption of the magnitude observed.
An atomistically informed mesoscale model for growth and coarsening during discharge in lithium-oxygen batteries
An atomistically informed mesoscale model is developed for the deposition of a discharge product in a Li-O{sub 2} battery. This mescocale model includes particle growth and coarsening as well as a simplified nucleation model. The model involves LiO{sub 2} formation through reaction of O{sub 2}{sup −} and Li{sup +} in the electrolyte, which deposits on the cathode surface when the LiO{sub 2} concentration reaches supersaturation in the electrolyte. A reaction-diffusion (rate-equation) model is used to describe the processes occurring in the electrolyte and a phase-field model is used to capture microstructural evolution. This model predicts that coarsening, in which large particles grow and small ones disappear, has a substantial effect on the size distribution of the LiO{sub 2} particles during the discharge process. The size evolution during discharge is the result of the interplay between this coarsening process and particle growth. The growth through continued deposition of LiO{sub 2} has the effect of causing large particles to grow ever faster while delaying the dissolution of small particles. The predicted size evolution is consistent with experimental results for a previously reported cathode material based on activated carbon during discharge and when it is at rest, although kinetic factors need to be included. The approach described in this paper synergistically combines models on different length scales with experimental observations and should have applications in studying other related discharge processes, such as Li{sub 2}O{sub 2} deposition, in Li-O{sub 2} batteries and nucleation and growth in Li-S batteries.
Aerosol samples obtained from 9-km to 12- km altitude
DC-8 aerosol sampling to determine spatial density of dust, and particle types and size distributions as functions of altitude and time
North Slope of Alaska Snow Intensive Operational Period Field Campaign Report
The campaign was motivated by the need to improve the quantification of measurements of ice-phase precipitation in the Arctic and was by the acquisition and deployment of the new X- and Ka/W-band radars. These radars opened up an opportunity for the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Climate Research Facility to obtain spatial estimates of snowfall rates using the polarimetric X-band measurements and dual-frequency measurements (using different combinations of the three wavelengths). However, calculations of X- and Ka-band radar back-scattering of ice crystal aggregates with their complex structure suggest that the commonly used T-matrix approach (Matrosov et al. 2007) for modeling the radar back-scattering underestimates the reflectivity by several decibels, with errors increasing with increasing radar frequency (Botta et al. 2010, 2011). Moreover, the X-band polarimetric measurements and the Ka/W-band measurements are sensitive to the assumed shape of the snow (Botta et al. 2011). One of the five ARM two-dimensional video disdrometers (manufactured by Joanneum Research) were deployed in Barrow at the ARM North Slope of Alaska (NSA) site from 1 October, 2011 to 31 May, 2012 in an attempt to use the instrument in a novel way. The instrument was originally designed to measure the drop size distribution of rain but it seemed worthwhile to explore its capability to quantify ice precipitation particle size and shape distributions in the cold north for scattering calculations and precipitation estimations. Furthermore, this deployment gave us an opportunity to see how reliable it could be in arctic conditions.
THE DUST ENVIRONMENT OF MAIN-BELT COMET P/2012 T1 (PANSTARRS)
The Main-Belt Comet P/2012 T1 (PANSTARRS) has been imaged using the 10.4 m Gran Telescopio Canarias and the 4.2 m William Herschel Telescope at six epochs in the period from 2012 November to 2013 February, with the aim of monitoring its dust environment. The dust tails' brightness and morphology are best interpreted in terms of a model of sustained dust emission spanning four to six months. The total dust mass ejected is estimated at {approx}6-25 Multiplication-Sign 10{sup 6} kg. We assume a time-independent power-law size distribution function, with particles in the micrometer to centimeter size range. Based on the quality of the fits to the isophote fields, an anisotropic emission pattern is favored against an isotropic one, in which the particle ejection is concentrated toward high latitudes ({+-}45 Degree-Sign to {+-}90 Degree-Sign ) in a high-obliquity object (I = 80 Degree-Sign ). This seasonally driven ejection behavior, along with the modeled particle ejection velocities, are in remarkable agreement to those we found for P/2010 R2 (La Sagra).