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DOE OSTI2020

A self-supervised workflow for particle picking in cryo-EM

High-resolution single-particle cryo-EM data analysis relies on accurate particle picking. To facilitate the particle picking process, a self-supervised workflow has been developed. This includes an iterative strategy, which uses a 2D class average to improve training particles, and a progressively improved convolutional neural network for particle picking. To automate the selection of particles, a threshold is defined (%/Res) using the ratio of percentage class distribution and resolution as a cutoff. This workflow has been tested using six publicly available data sets with different particle sizes and shapes, and can automatically pick particles with minimal user input. The picked particles support high-resolution reconstructions at 3.0 Å or better. This workflow is a step towards automated single-particle cryo-EM data analysis at the stage of particle picking. It may be used in conjunction with commonly used single-particle analysis packages such as Relion , cryoSPARC , cisTEM , SPHIRE and EMAN2 .

2D class averages↗

NASA NTRS1975

Diffraction analysis of Doppler signal characteristics for a cross-beam laser Doppler velocimeter

Based on scalar diffraction theory, single particle scattering characteristics for a cross-beam laser Doppler velocimeter (LDV) have been computed for different particle sizes under varied instrumentation configurations. The modulating component of the scattered signal has been shown to depend upon particle size, shape, and collecting aperture for a given probe volume fringe spacing. Experimental verifications of some of the predictions are presented, and some of the limitations using an LDV as a particle sizing instrument are discussed.

Robinson, D. M.↗

DOE OSTI2023

Electrochemical Characterization of Molten Salt Chemistry During Atmospheric Ingressions

This report describes the salt chemistry and sedimentation studies that were completed in FY23 as part of the Pyrochemical Fuel Cycles – ANL project. The primary objective of these activities was to employ electrochemical methods in order to quantify and gain insights into the reaction mechanisms associated with the interaction of O2 and moisture impurities with the molten chloride salts used for the pyrochemical processing of nuclear materials. If not monitored and controlled, the ingression of these atmospheric impurities can lead to changes in the salt redox conditions and initiate the formation of oxide particles, potentially resulting in operational and safeguards challenges. By elucidating the mechanisms underlying the formation of oxide particles, we can effectively monitor the conditions of the salt and design systems to mitigate the influence of atmospheric O2 and H2O. To achieve these goals, we designed a test system that allowed for precisely controlled gas ingressions into the molten salt vessel. This system included on-line monitoring provided by electrochemical probes that enable near real-time measurements of the salt conditions throughout the course of the experiment. Using this system, we systematically varied experimental conditions, including O2/Ar flow rates and O2 concentrations, to comprehensively understand their impact on solid particle formation. We also used a particle size and shape analyzer to characterize the particles that were generated. Tests in FY23 concentrated on the formation of CeO2 particles, but we also prepared a separate apparatus targeting UO2 particles for use in FY24. We additionally conducted extensive modeling activities in support of this work. This included multiphysics simulations of the gas ingressions along with the development of a machine learning workflow to enable accelerated molecular dynamics modeling of the molten salt chemistry of LiCl-KCl-UCl3. The combination of experimental and modeling tools has allowed us to begin to get a more complete understanding of the reactions that occur when atmospheric ingressions occur in pyroprocessing systems.

Guo, Jicheng↗

NASA NTRS2020

Wildfire Smoke Particle Properties and Evolution, From Space-Based Multi-Angle Imaging II: The Williams Flats Fire during the FIREX-AQ Campaign

Although the characteristics of biomass burning events and the ambient ecosystem determine emitted smoke composition, the conditions that modulate the partitioning of black carbon (BC) and brown carbon (BrC) formation are not well understood, nor are the spatial or temporal frequency of factors driving smoke particle evolution, such as hydration, coagulation, and oxidation, all of which impact smoke radiative forcing. In situ data from surface observation sites and aircraft field campaigns offer deep insight into the optical, chemical, and microphysical traits of biomass burning (BB) smoke aerosols, such as single scattering albedo (SSA) and size distribution, but cannot by themselves provide robust statistical characterization of both emitted and evolved particles. Data from the NASA Earth Observing System’s Multi-Angle Imaging SpectroRadiometer (MISR) instrument can provide at least a partial picture of BB particle properties and their evolution downwind, once properly validated. Here we use in situ data from the joint NOAA/NASA 2019 Fire Influence on Regional to Global Environments Experiment-Air Quality (FIREX-AQ) field campaign to assess the strengths and limitations of MISR-derived constraints on particle size, shape, light-absorption, and its spectral slope, as well as plume height and associated wind vectors. Based on the satellite observations, we also offer inferences about aging mechanisms effecting downwind particle evolution, such as gravitational settling, oxidation, secondary particle formation, and the combination of particle aggregation and condensational growth. This work builds upon our previous study, adding confidence to our interpretation of the remote-sensing data based on an expanded suite of in situ measurements for validation. The satellite and in situ measurements offer similar characterizations of particle property evolution as a function of smoke age for the 06 August Williams Flats Fire, and most of the key differences in particle size and absorption can be attributed to differences in sampling and changes in the plume geometry between sampling times. Whereas the aircraft data provide validation for the MISR retrievals, the satellite data offer a spatially continuous mapping of particle properties over the plume, which helps identify trends in particle property downwind evolution that are ambiguous in the sparsely sampled aircraft transects. The MISR data record is more than two decades long, offering future opportunities to study regional wildfire plume behavior statistically, where aircraft data are limited or entirely lacking.

biomass burning↗

DOE OSTI2023

Effects of Size and Shape on the Tolerances for Misalignment and Probabilities for Successful Oriented Attachment of Nanoparticles

Oriented attachment (OA) of nanoparticles is an important pathway of crystal growth, but tools for quantitatively modeling OA are lacking. Here we present several simple models that relate the probability of achieving OA to basic geometric parameters such as particle size, shape, and lattice periodicity. A Moiré-domain model is applied to understand twist-misorientations between parallel surfaces, and it predicts that the range of twist angles yielding perfect OA is inversely related to the width of the contact area. This is confirmed and further developed using a surface functional model, which predicts how crystallographic registration forces drive the emergence of complex orientational energy landscapes. The energy landscapes are predicted to possess local minima that can trap particles in imperfect alignments, and these local minima become deeper and more numerous as the contact area increases, making OA more challenging for large particles. Further, a second set of models is presented to understand the sequence of events by which two crystallographic faces become co-planer after collision. We use a ‘central force approximation’ to quantitatively predict the odds of attaining coalignment between various faces when particles collide with random misalignments, and we show that in the absence of biasing forces, the probability of attaining alignment on a given face is roughly proportional to its solid angle as viewed from the center of the particle. The model predicts that OA is most favorable between well-faceted particles and becomes exceedingly unlikely for large spherical particles that express many microfacets.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2022

Canadian and Alaskan Wildfire Smoke Particle Properties, Their Evolution and Controlling Factors, From Satellite Observations

The optical and chemical properties of biomass burning (BB) smoke particles greatly affect the impact that wildfires have on climate and air quality. Previous work has demonstrated some links between smoke properties and factors such as fuel type and meteorology. However, the factors controlling BB particle speciation at emission are not adequately understood nor are the factors driving particle aging during atmospheric transport. As such, modeling wildfire smoke impacts on climate and air quality remains challenging. The potential to provide robust, statistical characterizations of BB particles based on ecosystem type and ambient environmental conditions with remote sensing data is investigated here. Space-based Multi-angle Imaging SpectroRadiometer (MISR) observations, combined with the MISR Research Aerosol (RA) algorithm and the MISR Interactive Explorer (MINX) tool, are used to retrieve smoke plume aerosol optical depth (AOD) and to provide constraints on plume vertical extent; smoke age; and particle size, shape, light-absorption properties, and absorption spectral dependence. These tools are applied to numerous wildfire plumes in Canada and Alaska, across a range of conditions, to create a regional inventory of BB particle-type temporal and spatial distribution. We then statistically compare these results with satellite measurements of fire radiative power (FRP) and land cover characteristics, as well as short-term climate, meteorological, and drought information from the Modern-Era Retrospective analysis for Research and Applications (MERRA-2) reanalysis and the North American Drought Monitor. We find statistically significant differences in the retrieved smoke properties based on land cover type, with fires in forests producing the thickest plumes containing the largest, brightest particles and fires in savannas and grasslands exhibiting the opposite. Additionally, the inferred dominant aging mechanisms and the timescales over which they occur vary systematically between land types. This work demonstrates the potential of remote sensing to constrain BB particle properties and the mechanisms governing their evolution over entire ecosystems. It also begins to realize this potential, as a means of improving regional and global climate and air quality modeling in a rapidly changing world.

Katherine T. Junghenn Noyes↗

DOE OSTI2019

Shapes and Fall Orientations of Ice Particle Aggregates

Testing the often-made assumption that ice particle aggregates (snowflakes) are well represented by oblate spheroids, ellipsoid fits are applied to aggregate images. An algorithm to retrieve both the ellipsoidal parameters and the orientations of the fitted ellipsoids is applied to Multi-Angle Snowflake Camera measurements of ice particle aggregates observed in Alaska. The resulting ellipsoids have shapes closer to prolate spheroids than the oft-assumed oblate spheroids. A robust linear relationship exists between the two characteristic aspect ratios of the ellipsoids. The most probable orientation of the maximum dimension of the retrieved ellipsoids is not in the horizontal plane, and the rotational angles of the maximum dimensions in the horizontal plane are not uniform, but instead display some correlation with the wind direction at the times of the measurements. The retrieval results can be used to improve the representation of aggregates in microphysics and/or electromagnetic radiation scattering models applicable to radar and satellite measurements.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2019

Microphysical Retrievals from Simultaneous Measurements by Airborne and Ground Radars during OLYMPEX

The OLYMPEX field campaign took place over the Olympic Peninsula of Washington during winter 2015-2016. During the intensive observing period, several aircraft flights obtained multi-frequency airborne radar measurements at X-, Ku-, Ka, and W-band from radars aboard the ER-2 and DC-8 aircraft. In addition, ground radars at S- and X-band performed RHI scans under the aircraft ground tracks. These coincident datasets provide a wealth of complementary information about the hydrometeor particle sizes, shapes, and orientations.In order to synthesize these measurements and test the robustness of scattering models, an optimal estimation retrieval based upon a Hitschfeld-Bordan profiling algorithm has been developed. This algorithm retrieves profiles of the particle size distribution parameters Nw and Dm, and, in the ice phase, relative proportions of aggregate, pristine, and rimed particles, using scattering models with different size-density and size-aspect ratio relationships. Under this formulation, only the pristine particles are horizontally aligned and capable of producing non-zero ZDR and KDP.From the nadir-looking airborne multifrequency radars, we find that aggregates may be readily distinguished from rimed and pristine particles owing to their uniqueness in triple-frequency space. However, rimed and pristine particles occupy a similar region in this space and thus polarimetric measurements greatly enhance their identification in our retrieval framework. With these capabilities we will present analyses of three-dimensional hydrometeor mapping obtained during various OLYMPEX cases. Some features retrieved in these cases include a layer of enhanced aggregation about 2km above the melting layer, hypothesized to be maintained by orographic uplift. This layer is often situated above a layer of denser, aligned particles. Regions of riming and supercooled liquid water beneath generating cells are also identified by our retrieval algorithm. Comparisons to in-situ observations and evaluation of scattering models will be presented.

Munchak, S. Joseph↗

DOE OSTI2021

Use of Transmission Electron Microscopy for Analysis of Aerosol Particles and Strategies for Imaging Fragile Particles

For over 25 years, transmission electron microscopy (TEM) has provided a method for the study of aerosol particles with sizes from below the optical diffraction limit to several microns, resolving the particles as well as smaller features. The wide use of this technique to study aerosol particles has contributed important insights about environmental aerosol particle samples and model atmospheric systems. TEM produces an image that is a 2D projection of aerosol particles that have been impacted onto grids and, through associated techniques and spectroscopies, can contribute additional information such as the determination of elemental composition, crystal structure, and 3D particle structures. Soot, mineral dust, and organic/inorganic particles have all been analyzed using TEM and spectroscopic techniques. TEM, however, has limitations that are important to understand when interpreting data including the ability of the electron beam to damage and thereby change the structure and shape of particles, especially in the case of particles composed of organic compounds and salts. In this paper, we concentrate on the breadth of studies that have used TEM as the primary analysis technique. Another focus is on common issues with TEM and cryogenic-TEM. Insights for new users on best practices for fragile particles, that is, particles that are easily susceptible to damage from the electron beam, with this technique are discussed. Tips for readers on interpreting and evaluating the quality and accuracy of TEM data in the literature are also provided and explained.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2013

Orbiting Rainbows: Optical Manipulation of Aerosols and the Beginnings of Future Space Construction

Our objective is to investigate the conditions to manipulate and maintain the shape of an orbiting cloud of dust-like matter so that it can function as an ultra-lightweight surface with useful and adaptable electromagnetic characteristics, for instance, in the optical, RF, or microwave bands. Inspired by the light scattering and focusing properties of distributed optical assemblies in Nature, such as rainbows and aerosols, and by recent laboratory successes in optical trapping and manipulation, we propose a unique combination of space optics and autonomous robotic system technology, to enable a new vision of space system architecture with applications to ultra-lightweight space optics and, ultimately, in-situ space system fabrication. Typically, the cost of an optical system is driven by the size and mass of the primary aperture. The ideal system is a cloud of spatially disordered dust-like objects that can be optically manipulated: it is highly reconfigurable, fault-tolerant, and allows very large aperture sizes at low cost. See Figure 1 for a scenario of application of this concept. The solution that we propose is to construct an optical system in space in which the nonlinear optical properties of a cloud of micron-sized particles are shaped into a specific surface by light pressure, allowing it to form a very large and lightweight aperture of an optical system, hence reducing overall mass and cost. Other potential advantages offered by the cloud properties as optical system involve possible combination of properties (combined transmit/receive), variable focal length, combined refractive and reflective lens designs, and hyper-spectral imaging. A cloud of highly reflective particles of micron-size acting coherently in a specific electromagnetic band, just like an aerosol in suspension in the atmosphere, would reflect the Sun's light much like a rainbow. The only difference with an atmospheric or industrial aerosol is the absence of the supporting fluid medium. This new concept is based on recent understandings in the physics of optical manipulation of small particles in the laboratory and the engineering of distributed ensembles of spacecraft clouds to shape an orbiting cloud of micron-sized objects. In the same way that optical tweezers have revolutionized micro- and nano-manipulation of objects, our breakthrough concept will enable new large scale NASA mission applications and develop new technology in the areas of Astrophysical Imaging Systems and Remote Sensing because the cloud can operate as an adaptive optical imaging sensor. While achieving the feasibility of constructing one single aperture out of the cloud is the main topic of this work, it is clear that multiple orbiting aerosol lenses could also combine their power to synthesize a much larger aperture in space to enable challenging goals such as exoplanet detection. Furthermore, this effort could establish feasibility of key issues related to material properties, remote manipulation, and autonomy characteristics of cloud in orbit. There are several types of endeavors (science missions) that could be enabled by this type of approach, i.e. it can enable new astrophysical imaging systems, exoplanet search, large apertures allow for unprecedented high resolution to discern continents and important features of other planets, hyperspectral imaging, adaptive systems, spectroscopy imaging through limb, and stable optical systems from Lagrange-points. Future micro-miniaturization might hold promise of a further extension of our dust aperture concept to other more exciting smart dust concepts with other associated capabilities.

Space Construction↗

NASA NTRS1972

The shape of the interstellar reddening law

The spectral distribution of pairs of stars within the same spectral type and luminosity class, one of which is reddened and the other unreddened is compared. It is assumed that the observed difference between two stars is only attributed to the interstellar medium. Their physical properties, size distribution of particles, geometrical shape, and their location in space are considered.

Laget, M.↗

NASA NTRS2011

Monitoring Aerosols from Space: What We can Say, and What We Can't

Aerosols are understood to play a significant role is the global energy balance, and especially on atmospheric as well as surface energy balances regionally. A combination of direct radiative cooling of the surface, atmospheric warming through diabatic heating, and indirect effects of aerosol on clouds are all thought to contribute to the net aerosol effect, though the magnitudes of each are both highly variable in space and time, and highly uncertain. Passive space-based remote sensing is a key tool for constraining these effects, due to the frequent, global coverage satellites can provide. However, information from such observations about total-column aerosol amount (i.e., aerosol optical depth or AOD), and especially about aerosol type, is limited. The current generation of passive aerosol remote-sensing instruments, including the Multi-angle Imaging SpectroRadiometer (MISR) and the MODerate resolution Imaging Spectroradiometer (MODIS) offer vast improvements over previous instruments, including AOD over water and much of the land surface, fine vs. coarse particle type over ocean from MODIS, and discrimination of about a dozen aerosol types from MISR under good retrieval conditions, based on particle size, shape, and single-scattering albedo (SSA) constraints. This presentation will summarize the capabilities and expected improvements in the currently available aerosol products, in light of required energy budget constraints. Ways of addressing the need for detailed information about particle microphysical properties, especially SSA, unobtainable from MISR or MODIS, will be discussed.

Kahn, Ralph A.↗

NASA NTRS2012

Steps Toward an EOS-Era Aerosol Type Climatology

We still have a way to go to develop a global climatology of aerosol type from the EOS-era satellite data record that currently spans more than 12 years of observations. We have demonstrated the ability to retrieve aerosol type regionally, providing a classification based on the combined constraints on particle size, shape, and single-scattering albedo (SSA) from the MISR instrument. Under good but not necessarily ideal conditions, the MISR data can distinguish three-to-five size bins, two-to-four bins in SSA, and spherical vs. non-spherical particles. However, retrieval sensitivity varies enormously with scene conditions. So, for example, there is less information about aerosol type when the mid-visible aerosol optical depth (AOD) is less that about 0.15 or 0.2, or when the range of scattering angles observed is reduced by solar geometry, even though the quality of the AOD retrieval itself is much less sensitive to these factors. This presentation will review a series of studies aimed at assessing the capabilities, as well as the limitations, of MISR aerosol type retrievals involving wildfire smoke, desert dust, volcanic ash, and urban pollution, in specific cases where suborbital validation data are available. A synthesis of results, planned upgrades to the MISR Standard aerosol algorithm to improve aerosol type retrievals, and steps toward the development of an aerosol type quality flag for the Standard product, will also be covered.

Kahn, Ralph A.↗

NASA NTRS2012

Steps Toward an EOS-Era Aerosol Air Mass Type Climatology

Kahn, Ralph A.↗

NASA NTRS1993

Study on the mechanism of liquid phase sintering (M-12)

The objectives were to (1) obtain the data representing the growth rate of solid particles in a liquid matrix without the effect of gravity; and (2) reveal the growth behavior of solid particles during liquid phase sintering using the data obtained. Nickel and tungsten are used as the constituent materials in liquid phase sintering. The properties of the constituent metals are given. When a compact of the mixture of tungsten and nickel powders is heated and kept at 1550 C, nickel melts down but tungsten stays solid. As the density of tungsten is much greater than that of nickel, the sedimentation of tungsten particles occurs in the experiment on Earth. The difference between the experiments on Earth and in space is illustrated. The tungsten particles sink to the bottom and are brought into contact with each other. The resulting pressure at the contact point causes the accelerated dissolution of tungsten. Consequently, flat surfaces are formed at the contact sites. As a result of dissolution and reprecipitation of tungsten, the shape of particles changes to a polygon. This phenomenon is called 'flattening.' An example of flattening of tungsten particles is shown. Thus, the data obtained by the experiment on Earth may not represent the exact growth behavior of the solid particles in a liquid matrix. If the experiments were done in a microgravity environment, the data corresponding to the theoretical growth behavior of solid particles could be achieved.

Kohara, S.↗

NASA NTRS2020

The Evolution of Icelandic Volcano Emissions, as Observed From Space in the Era of NASA's Earth Observing System (EOS)

Volcanoes are natural phenomena that have global environmental impacts. Satellite remote sensing can help classify volcanic eruptions and track the dispersion of emissions. We assess multiple volcanic eruptions in Iceland (Eyjafjallajökull 2010, Grímsvötn 2011 and Holuhraun 2014-2015), using space-borne observations to infer information about the geological dynamics of each volcano and the properties and evolution of plume particles. We derive qualitative constraints on plume particle size, shape and light-absorption characteristics from Multi-angle Imaging SpectroRadiometer (MISR) space-borne imagery. With the MISR Research Algorithm (RA), we distinguish sulfate/water-dominated volcanic plumes from Holuhraun and ash-dominated plumes from Eyjafjallajökull and Grímsvötn, and even identify subtler changes in ash particle size and light-absorption within plumes. Additionally, plume heights are retrieved geometrically from MISR. These are combined with surface thermal anomalies from the MODerate resolution Imaging Spectroradiometer (MODIS) and SO2 concentrations derived from the Ozone Monitoring Instrument (OMI) to synthesize eruption remote-sensing chronologies. Signals related to differences in particle properties are identified and linked to evolving magma composition at Eyjafjallajökull. The results illustrate the potential to distinguish qualitative differences in eruptive magma composition based on particle light absorption and plume profile from remote-sensing. For the sulfate-rich Holuhraun plumes, the influence of aerosol hygroscopic growth during transport is inferred from such data. Three processes appear to dominate plume evolution in Iceland: downwind aerosol formation; particle hydration; and particle deposition. This work demonstrates enhanced MISR capabilities, and more generally, remote-sensing analysis that can be applied globally, especially where suborbital volcano observations are limited or entirely absent.

remote sensting↗

NASA NTRS2011

Packing Optimization of Sorbent Bed Containing Dissimilar and Irregular Shaped Media

The Fire Cartridge is a packed bed air filter with two different and separate layers of media designed to provide respiratory protection from combustion products after a fire event on the International Space Station (ISS). The first layer of media is a carbon monoxide catalyst and the second layer of media is universal carbon. During development of Fire Cartridge prototypes, the two media beds were noticed to have shifted inside the cartridge. The movement of media within the cartridge can cause mixing of the bed layers, air voids, and channeling, which could cause preferential air flow and allow contaminants to pass through without removal. An optimally packed bed mitigates these risks and ensures effective removal of contaminants from the air. In order to optimally pack each layer, vertical, horizontal, and orbital agitations were investigated and a packed bulk density was calculated for each method. Packed bulk density must be calculated for each media type to accommodate variations in particle size, shape, and density. Additionally, the optimal vibration parameters must be re-evaluated for each batch of media due to variations in particle size distribution between batches. For this application it was determined that orbital vibrations achieve an optimal pack density and the two media layers can be packed by the same method. Another finding was media with a larger size distribution of particles achieve an optimal bed pack easier than media with a smaller size distribution of particles.

Holland, Nathan↗

NASA NTRS1994

Comet coma sample return instrument

The sample collection technology and instrument concept for the Sample of Comet Coma Earth Return Mission (SOCCER) are described. The scientific goals of this Flyby Sample Return are to return to coma dust and volatile samples from a known comet source, which will permit accurate elemental and isotopic measurements for thousands of individual solid particles and volatiles, detailed analysis of the dust structure, morphology, and mineralogy of the intact samples, and identification of the biogenic elements or compounds in the solid and volatile samples. Having these intact samples, morphologic, petrographic, and phase structural features can be determined. Information on dust particle size, shape, and density can be ascertained by analyzing penetration holes and tracks in the capture medium. Time and spatial data of dust capture will provide understanding of the flux dynamics of the coma and the jets. Additional information will include the identification of cosmic ray tracks in the cometary grains, which can provide a particle's process history and perhaps even the age of the comet. The measurements will be made with the same equipment used for studying micrometeorites for decades past; hence, the results can be directly compared without extrapolation or modification. The data will provide a powerful and direct technique for comparing the cometary samples with all known types of meteorites and interplanetary dust. This sample collection system will provide the first sample return from a specifically identified primitive body and will allow, for the first time, a direct method of matching meteoritic materials captured on Earth with known parent bodies.

Albee, A. L.↗