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X-Ray Microtomography Measurements of Coevolving Particle Size and Shape

This study measures simultaneous changes in particle size and shape during grain crushing and proposes quantitative metrics to track their coevolving statistical distribution. Idealized granular materials with widely different initial particle shapes (i.e., spheres, quasi-ellipsoids, plates, and rods) are compressed oedometrically at vertical stress levels sufficient to induce particle breakage. X-ray microtomography and digital image analysis are then used to track changes in particle-scale characteristics. The observations indicate that more irregular particles tend to exhibit a higher degree of breakage compared to more spherical grains subjected to an equivalent stress level. Despite these differences, the measurements also indicate that all the tested particle sets approach a common attractor (expressed in terms of aspect ratio, flatness, and elongation), regardless of their initial morphology. A new shape evolution index is proposed to quantify such trends. With this new metric, it is shown that in all the tested materials, the particle shape evolves faster than size, especially for the more regular morphologies, thus implying that the shape tends to reach its attractor point before the grading reaches its ultimate particle size distribution. Furthermore, this finding underpins an ultimate stage of crushing-driven compression that occurs with particle size reduction but minimal shape changes (i.e., self-replicating shapes due to fractures).

Oedometric compression↗

Mineral Dust Cycle in the Multiscale Online Nonhydrostatic AtmospheRe CHemistry Model (Monarch) Version 2.0

We present the dust module in the Multiscale Online Non-hydrostatic AtmospheRe CHemistry model (MONARCH) version 2.0, a chemical weather prediction system that can be used for regional and global modeling at a range of resolutions. The representations of dust processes in MONARCH were upgraded with a focus on dust emission (emission parameterizations, entrainment thresholds, considerations of soil moisture and surface cover), lower boundary conditions (roughness, potential dust sources), and dust–radiation interactions. MONARCH now allows modeling of global and regional mineral dust cycles using fundamentally different paradigms, ranging from strongly simplified to physics-based parameterizations. We present a detailed description of these updates along with four global benchmark simulations, which use conceptually different dust emission parameterizations, and we evaluate the simulations against observations of dust optical depth. We determine key dust parameters, such as global annual emission/deposition flux, dust loading, dust optical depth, mass-extinction efficiency, single-scattering albedo, and direct radiative effects. For dust-particle diameters up to 20 µm, the total annual dust emission and deposition fluxes obtained with our four experiments range between about 3500 and 6000 Tg, which largely depend upon differences in the emitted size distribution. Considering ellipsoidal particle shapes and dust refractive indices that account for size-resolved mineralogy, we estimate the global total (longwave and shortwave) dust direct radiative effect (DRE) at the surface to range between about −0.90 and −0.63 W m−2 and at the top of the atmosphere between −0.20 and −0.28 W m−2. Our evaluation demonstrates that MONARCH is able to reproduce key features of the spatiotemporal variability of the global dust cycle with important and insightful differences between the different configurations.

Dust cycle↗

In situ measurement of particulate number density and size distribution from an aircraft

Commercial particulate measuring instruments were flown aboard the NASA Convair 990. A condensation nuclei monitor was utilized to measure particles larger than approximately 0.003 micrometers in diameter. A specially designed pressurization system was used with this counter so that the sample could be fed into the monitor at cabin altitude pressure. A near-forward light scattering counter was used to measure the number and size distribution particles in the size range from 0.5 to 5 micrometers and greater in diameter.

Briehl, D.↗

The effect of alloy composition on the mechanism of stress-corrosion cracking of titanium alloys in aqueous environments

A detailed study was made of the relation between the size distribution of Ti3Al particles in a Ti-8Al alloy and the tensile properties measured in air and in saltwater. The size distribution of Ti3Al was varied by isothermal aging for various times at temperatures in the range 770 to 970 K (930 to 1290 F). The aging kinetics were found to be relatively slow. Quantitative measurements of the particle coarsening rate at 920 K (1200 F) showed good agreement with the predicted behavior for coarsening controlled by matrix diffusion, and suggested that the specific free energy of the Ti3Al alpha interface in negligible small. In all cases, the Ti3Al particles were sheared by the glide dislocations. It was concluded that there is a definite correlation between the presence of deformable Ti3Al particles and an alloy's susceptibility to aqueous stress corrosion cracking. Furthermore, the appearance of the surface slip lines and the dislocation substructure in deformed specimens suggest that the specific effect of the Ti3Al particles is to cause a nonhomogeneous planar slip character and an enhanced chemical potential of the slip bands.

Wood, R. A.↗

Dynamic Light Scattering With Improved Fiber-Optic Probes

Improved fiber-optic probes developed for use in dynamic light-scattering measurements. Intended for measuring dynamic backscattering of laser light from concentrated suspensions of particles in liquids, for purpose of determining statistical distributions of sizes of particles. Offers advantages of compactness and ruggedness, and more suitable for industrial environments. Probes immersed in suspensions characterized. Associated lasers, photodetectors, and signal-processing circuits located remotely in safer environments, coupled to probes via optical fibers.

Dhadwal, Harbans Singh↗

Using Dust from Asteroids as Regolith Microsamples

More robust links need to be forged between meteorites and their parent bodies to understand the composition, diversity and distribution of the asteroids. A major link can be sample analysis of the parent body material and comparison with meteorite data. Dust is present around all airless bodies, generated by micrometeorite impact into their airless surfaces, which in turn lofts regolith particles into a "cloud" around the body. The composition, flux, and size distribution of dust particles can provide insight into the geologic evolution of airless bodies. For example, the Cassini Cosmic Dust Analyzer detected salts and minerals emitted by plumes at Enceladus, evidence for a subsurface ocean with a silicate seafloor. Dust analysis instruments may enable future missions to obtain elemental, isotopic and mineralogical composition of regolith particles without returning the samples to terrestrial laboratories.

dust↗

Quantifying structural errors in cloud condensation nuclei activity from reduced representation of aerosol size distributions

Aerosol effects on clouds and radiation are the dominant contribution to uncertainty in radiative forcing relative to the pre-industrial atmosphere. While previous studies have assessed the impact of parametric uncertainty on modeled forcing, structural errors from the numerical representation of particle distributions have not been well quantified. Here we present a framework for quantifying error in aerosol size distributions and cloud condensation nuclei activity, which we apply to the widely used 4-mode version of the Modal Aerosol Module (MAM4). Box model predictions from the MAM4 are evaluated against the Particle Monte Carlo Model for Simulating Aerosol Interactions and Chemistry (PartMC-MOSAIC), a benchmark model that tracks the evolution of individual particles. We show that size distributions simulated by MAM4 diverge from those simulated by PartMC-MOSAIC after only a few hours of aging by condensation and coagulation in polluted conditions, which leads to large errors in modeled cloud condensation nuclei concentrations. We find that differences between MAM4 and PartMC-MOSAIC are largest under polluted conditions, where the size distribution evolves rapidly though aging by condensation of semi-volatile substances and coagulation among particles. These findings suggest that structural error in modeled aerosol properties contributes to the large inter-model variability in aerosol radiative forcing.

Fierce, Laura M.↗

Expected characteristics of large dust particles in periodic Comet Halley

Observational evidence is presented for dust particles heavier than 0.01 millionth of a gram expelled from Comet Halley. Dust emitted around 1.5 AU pre-perihelion, the point in orbit where a probe would fly through the comet in 1985, should have contributed to an anomalous tail that could have been observed in 1910. From positions of the trailing boundary of the ordinary dust tail at that time, it is concluded that the production of dust started to increase steeply at 0.7 to 0.8 AU before perihelion. Observations in late January 1836 are used to derive the production of dust vs. time and the the expected number of large-particle impacts on the protective shield of the 1985 flythrough probe. From data on other comets, it is estimated that the size distribution for large particles is likely to vary inversely according to the fourth or slightly higher power of the size.

Sekanina, Z.↗

Multiscale modeling of packed-bed microwave reactors and estimation of intrinsic materials' permittivity

Modeling of packed-bed microwave reactors relies on an accurate representation of particle size, shape, and distribution within the bed, as well as the particles' dielectric properties. The measured permittivity of microwave susceptors (powders or structured materials) depends on the geometric features of the particles and the porosity of the bed, as well as the specific form factor of a structured material. These are effective properties and cannot be used to analyze other reactor configurations unless the geometric effects are removed. Therefore, we introduce a methodology for extracting the intrinsic particle permittivity from experimentally measured effective permittivity by combining cavity-based measurements with multiscale simulations and machine learning. Further, we develop the first multiscale model of packed-bed microwave reactors that incorporate particle effects (geometric features, random packing, and particle contact). This approach bridges macroscopic observables with mesoscopic physics, enabling analysis of local hotspots, arcing, and contact effects that control reactor performance. Using polymer-based spherical activated carbon (PBSAC) and silicon carbide (SiC) as examples, we demonstrate that the inferred particle permittivity is consistent with independent experimental heating profiles we collect from microwave reactors without adjustable parameters. Finally, this methodology establishes a foundation for predictive, multiscale design of microwave packed-bed reactors that explicitly accounts for particle-scale effects, enabling the estimation of intrinsic permittivity for the first time.

97 MATHEMATICS AND COMPUTING↗

AERACEPT (Aerosol Rapid Analysis Combined Entry Probe/sonde Technology): Enabling Technology for Missions to the Venus Clouds

AERACEPT (AErosol Rapid Analysis Combined Entry Probe/sonde Technology) is an early-stage technology allowing a single aeroshell body to act as both an entry vehicle and aerosol-sampling passive descent sonde. AERACEPT does not require heat shield separation, deployable parachutes, or descent control, thus reducing the mass, volume, and complexity of planetary aerosol sampling. AERACEPT is particularly well suited for a Venus mission, where the particles of greatest interest are within the subsonic descent regime. AERACEPT uses the aeroshell’s own velocity to drive aerosol capture and separation through a series of embedded inlets. It takes advantage of recently developed thermal protection materials (3D-CC and HEEET) in combination with heritage aerosol sampling technologies from both planetary and airborne science (high-speed inlets and particle separation). The trade space for a given descent trajectory includes the particle capture efficiency for a given size, the bias introduced in the sampled particle size and concentration distributions, and the thermal alteration experienced by the particles during their brief exposure to the internal flow environment. AERACEPT is included in the Nephele mission concept study for a small spacecraft targeting the Venus middle and lower cloud layers. Nephele complements larger missions targeting Venus atmospheric gas analysis, such as DAVINCI and Venera-D, by specifically targeting cloud and haze particles. Because of the short lifetime of the probe in the lower atmosphere, Nephele requires a fast cadence of analysis of the captured particles, and includes the VOLTR dual optical spectrometer (SERS/LIBS) as part of its notional payload. Preliminary modeling based on the Nephele trajectory at 63 km to 39 km indicates AERACEPT can limit sample heating to 30-60 K above ambient. A modified particle tracking model has been implemented to estimate capture efficiency of particles larger than 0.1 µm and total sample volume as part of an inlet and interal flow path geometry trade study. Further modeling and empirical testing is underway to improve these estimates.

AERACEPT↗

Measurement of flow properties coupled to experimental and numerical analyses of dense, granular flows for solar thermal energy storage

Granular flows of sintered bauxite proppants were researched along an inclined plane for solar thermal energy storage applications. Granular flow properties needed to drive numeric granular models were measured for improved numerical model predictions for Carbobead CP 50/140, 40/100, and 30/60 particles. Particle shape and size distributions were determined by coupling optical microscopy to an in-house image processing algorithm. The impulse excitation technique was used to measure elastic and shear moduli, and compute Poisson’s ratio. The coefficient of static sliding friction was measured using the slip-stick method, and the static rolling friction was determined from measured shear on particles positioned between two hot-pressed plates. The coefficient of restitution was measured by dropping particles on a surface and determining the kinetic energy before and after impact with the surface using high resolution particle tracking velocimetry. Particle size did not significantly impact the coefficients of restitution and static rolling friction, however, particle shape distribution resulted in a large variation in measurements. An inclined flow experiment was performed to characterize granular flows of Carbobead CP 30/60 particles using particle image velocimetry. Numerical models of the experiment using discrete element method were generated with the measured mechanical properties as inputs for comparison with experimental results. A constant directional torque rolling friction model best predicted bulk granular flow behavior. Furthermore, good agreement between the model and experiment was achieved at ambient, steady state conditions, with average velocity differences <10%.

14 SOLAR ENERGY↗

A Sensitivity Study on the Effects of Particle Chemistry, Asphericity and Size on the Mass Extinction Efficiency of Mineral Dust in the Earth's Atmosphere: From the Near to Thermal IR

To determine a plausible range of mass extinction efficiencies (MEE) of terrestrial atmospheric dust from the near to thermal IR, sensitivity analyses are performed over an extended range of dust microphysical and chemistry perturbations. The IR values are subsequently compared to those in the near-IR, to evaluate spectral relationships in their optical properties. Synthesized size distributions consistent with measurements, model particle size, while composition is defined by the refractive indices of minerals routinely observed in dust, including the widely used OPAC/Hess parameterization. Single-scattering properties of representative dust particle shapes are calculated using the T-matrix, Discrete Dipole Approximation and Lorenz-Mie light-scattering codes. For the parameterizations examined, MEE ranges from nearly zero to 1.2 square meters per gram, with the higher values associated with non-spheres composed of quartz and gypsum. At near-IR wavelengths, MEE for non-spheres generally exceeds those for spheres, while in the thermal IR, shape-induced changes in MEE strongly depend on volume median diameter (VMD) and wavelength, particularly for MEE evaluated at the mineral resonant frequencies. MEE spectral distributions appear to follow particle geometry and are evidence for shape dependency in the optical properties. It is also shown that non-spheres best reproduce the positions of prominent absorption peaks found in silicates. Generally, angular particles exhibit wider and more symmetric MEE spectral distribution patterns from 8-10 micrometers than those with smooth surfaces, likely due to their edge-effects. Lastly, MEE ratios allow for inferring dust optical properties across the visible-IR spectrum. We conclude the MEE of dust aerosol are significant for the parameter space investigated, and are a key component for remote sensing applications and the study of direct aerosol radiative effects.

Hansell, R. A., Jr.↗

Mixing states of Amazon basin aerosol particles transported over long distances using transmission electron microscopy

The Amazon basin is important for understanding the global climate because of its carbon cycle and as a laboratory for obtaining basic knowledge of the continental background atmosphere. Aerosol particles play an important role in the climate and weather, and knowledge of their compositions and mixing states is necessary to understand their influence on the climate. For this study, we collected aerosol particles from the Amazon basin during the Green Ocean Amazon (GoAmazon2014/5) campaign (February to March 2014) at the T3 site, which is located about 70 km from Manaus, and analyzed them using transmission electron microscopy (TEM). TEM has better spatial resolution than other instruments, which enables us to analyze the occurrences of components that attach to or are embedded within other particles. Based on the TEM results of more than 10 000 particles from several transport events, this study shows the occurrences of individual particles including compositions, size distributions, number fractions, and possible sources of materials that mix with other particles. Aerosol particles during the wet season were from both natural sources such as the Amazon forest, Saharan desert, Atlantic Ocean, and African biomass burning and anthropogenic sources such as Manaus and local emissions. These particles mix together at an individual particle scale. The number fractions of mineral dust and sea-salt particles increased almost 3-fold when long-range transport (LRT) from the African continent occurred. Nearly 20 % of mineral dust and primary biological aerosol particles had attached sea salts on their surfaces. Sulfates were also internally mixed with sea-salt and mineral dust particles. The TEM element mapping images showed that several components with sizes of hundreds of nanometers from different sources commonly occur within individual LRT aerosol particles. We conclude that many aerosol particles from natural sources change their compositions by mixing during transport. The compositions and mixing states of these particles after emission result in changes in their hygroscopic and optical properties and should be considered when assessing their effects on climate.

54 ENVIRONMENTAL SCIENCES↗

Mixing states of Amazon-basin aerosol particles transported over long distances using transmission electron microscopy

The Amazon basin is important for understanding the global climate both because of its carbon cycle and as a laboratory for obtaining basic knowledge of the continental background atmosphere. Aerosol particles play an important role in the climate and weather, and knowledge of their compositions and mixing states is necessary to understand their influence on the climate. For this study, we collected aerosol particles from the Amazon basin during the Green Ocean Amazon (GoAmazon2014/5) campaign (February to March 2014) at the T3 site, which locates about 70 km from Manaus, and analyzed using transmission electron microscopy (TEM). TEM has better spatial resolution than other instruments, which enables us to analyse the occurrences of components that attach to or are embedded within other particles. Based on the TEM results of more than 10,000 particles from several transport events, this study shows the occurrences of individual particles including compositions, size distributions, number fractions, and possible sources of materials that mix with other particles. Aerosol particles during the wet season were from both natural sources such as the Amazon forest, Saharan desert, Atlantic Ocean, and African biomass burning and anthropogenic sources such as Manaus and local emissions. These particles mix together at an individual particle scale. The number fractions of mineral dust and sea-salt particles increased almost three-fold when long-range transport (LRT) from the African continent occurred. Nearly 20 % of mineral dust and primary biological aerosol particles attached sea salts on their surfaces. Sulfates were also internally mixed with sea-salt and mineral dust particles. The TEM element mapping images showed that several components with sizes of hundreds of nanometres from different sources commonly occur within individual LRT aerosol particles. We conclude that many aerosol particles from natural sources change their compositions by mixing during transport. The compositions and mixing states of these particles after emission result in changes in their hygroscopic and optical properties and should be considered when assessing their effects on climate.

54 ENVIRONMENTAL SCIENCES↗

Artifacts in the Aerosol Size Distribution Measured by the Ultra-High-Sensitivity Aerosol Spectrometer (UHSAS)

The ultra-high-sensitivity aerosol spectrometer (UHSAS) (Droplet Measurement Technologies, Longmont, Colorado) is an optical particle size spectrometer that determines aerosol size distributions in the diameter range from 60 to 1000 nm in 100 logarithmically spaced diameter bins1 by measuring the amount of light scattered by individual aerosol particles from a 1054-nm laser. Recently, it was noticed that aerosol size distributions determined by the UHSAS from all U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility sites exhibited modes at diameters greater than ~500 nm (Figure 1, blue arrows). These modes were not present in size distributions determined by another aerosol spectrometer that was co-located with the UHSAS, the Grimm 11D optical particle counter (OPC) (GRIMM Aerosol Technik Ainring GmbH & Co. KG, Germany), which sizes particles into 31 linearly spaced diameters bins from 253 to 35,150 nm using a 683-nm wavelength laser. Additionally, abrupt changes in aerosol particle number concentration with changing particle diameter are seen in UHSAS data at several diameters (Figure 1, red arrows). The purpose of this report is to explain the origin of the modes and the abrupt changes in aerosol size distributions observed by the UHSAS and why they are absent in the data from the Grimm OPC.

54 ENVIRONMENTAL SCIENCES↗

Optical Scattering Characterization for the Glennan Microsystems Microscale Particulate Classifier

Small sensors that are tolerant to mechanically and thermally harsh environments present the possibility for in-situ particle characterization in propulsion, industrial, and planetary science applications. Under a continuing grant from the Glennan Microsystems Initiative to the Microgravity Fluids Physics Branch of the NASA-Glenn Research Center, a Microscale Particle Classifier (MiPAC) instrument is being developed. The MiPAC instrument will be capable of determining the size distribution of airborne particles from about 1 nm to 30 micrometers, and will provide partial information as to the concentration, charge state, shape, and structure of the particles, while being an order of magnitude smaller in size and lighter in weight than presently commercially available instruments. The portion of the instrument that will characterize the nm-range particles will employ electrical mobility techniques and is being developed under a separate grant to Prof. David Pui of the University of Minnesota. The portion of the instrument that will characterize the micrometer-size particles such as dirt, pollens, spores, molds, soot, and combustion aerosols will use light scattering techniques. The development of data analysis techniques to be employed in the light scattering portion of the instrument is covered by this grant.

Lock, James A.↗

When and Where Lithium Plating Occurs, Its Correlation with Microstructure Heterogeneity, and the Mechanisms That Initiate and Self-Regulate Electrochemical Heterogeneity (A02-0444)

A microstructure scale electrochemical LIB model was used to investigate lithium plating onset, material non-uniform utilization, and in-plane heterogeneities for an NMC-graphite full cell. Model predicts active material particle surface roughness and size distribution (respectively, non-uniform curvature within and between particles) initiate in-plane heterogeneity, and that particle size heterogeneity at the separator interface controls the lithium plating preferential deposition ("Where"). These in-plane heterogeneities are then exacerbated by through-plane heterogeneities induced at fast charge as electrolyte depletion occurs and concentrates intercalation reaction near the anode-separator interface. Also, magnitude and occurrence of lithium plating is controlled by effective, or macroscale, microstructure parameters ("When"). As local states of charge start to diverge between nearby active material regions, overpotential differences induced by OCP difference kick in and contribute to reduce these SOC local heterogeneities. However, for staged materials such as graphite, with OCP profile alternating between plateaus and varying regions, this balancing mechanism is, respectively, inactive and active. This leads to a dynamic, non-monotonic, in-plane heterogeneity time evolution for state of charge and Faraday current density, for which their respective in-plane heterogeneity magnitude alternates. Such behavior has been modeled both for the whole electrode at the microstructure scale and at the particle scale. In-plane heterogeneities are usually considered to be detrimental, as they result in material non-uniform utilization (i.e., under and over stressed regions) and earlier degradations. However, this work provides a more granular approach as it discriminates between a harmful in-plane heterogeneity (non-uniform curvature) that triggers SOC in-plane heterogeneity, and a beneficial in-plane heterogeneity (Faraday current density) that contributes to reduce SOC in-plane heterogeneity. This work comprehensively explains the mechanisms that initiate, exacerbate, and regulate heterogeneity at the microstructure scale, while providing some design suggestions to reduce both in-plane and through-plane heterogeneities, as summarized in the graphical abstract.

ADVANCED PROPULSION SYSTEMS↗

A New Look Into the Treatment of Large Drops in Radiative Transfer

One of the weakest links in conventional cloud radiation models is the way a size distribution of cloud particles is mathematically handled: one averages measured drop concentrations over space, evaluates the extinction and scattering cross sections using the mean drop size distribution function and solves the radiative transfer equation with average characteristics. This technique assumes that all drop sizes are well represented in ary given interval along the direction of photon travel. But the concentration of large drops can be so law that this assumption is significantly violated. This is clearly seen if one examines of how the appearance of drops changes with the scale. In the poster we demonstrate the results of our analysis of FSSP data acquired during FIRE'87 and both FSSP and DC1 data from cloud IOP in Spring 2000. The analysis shows that, in general, the average number of drops observed in an interval along the direction of photon travel is proportional to the interval's length (or scale) powered to a drop scaling exponent. For small droplets the scaling exponent is equal to 1, as predicted by a conventional radiative transfer model. However, for large drops, the scaling exponent can fall distinctly below 1. Since the solution of radiative transfer equation depends on the drop scaling exponent, its deviation from unity can lead to a systematic bias in estimation of cloud radiative properties. We discuss the importance of the scaling exponent for the characteristics of the small-scale drop size variability for large and small droplets. Most of the existing cloud radiation models, however, are insensitive to this parameter.

Marshak, Alexander↗