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DOE OSTI2023

Assessing the link between aerosol mixing state, structure and composition and their optical properties: Ascension Island as a testbed for the South‐East Atlantic aerosol regimes

Forest and savanna fires are a major source of pollution over the globe. Such fire events emit to the atmosphere a considerable amount of “fluffy” fractal black looking particles that are often referred to as black carbon (BC) or soot aerosols. In fact, BC particles (aerosols) emitted from savanna and agricultural fires over the African continent play an important role in the region’s and the global climate. These fires occur each year between July and October, which is referred to as the biomass burning (BB) season and are considered among the globe's largest man-made emission sources of BC particles. However, during these fire events, not only BC particles are emitted, but also other types of particles and gases that can interact with each other to create new particles, generating a slew of particles often generally referred to as BB aerosols. Although the majority of the fire emissions occur inland in the sub-Saharan part of Africa, their effect reaches far beyond the continent due to the prevailing easterly winds, which transport those aerosols over the South-East Atlantic (SEA) ocean, off the west-coast of Africa. The reason why these particles are so important to the regional and global climate is that they absorb sunlight radiation, which overall warms the climate. However, the magnitude of this warming effect is highly uncertain and depends upon a multitude of aspects. Our overarching goal for this project was to better understand the changes in the aerosol properties as they transport from fire sources downstream toward the ocean and how this can eventually affect the earth's radiative budget in terms of warming or cooling. Following the above, our work here was focused on the investigation of the African BB aerosol plumes mixing state (mixing of BB aerosols and other aerosol types), composition and size distribution as they transport from the African continent towards the SEA ocean, and their link with some of the commonly measurable bulk optical properties such as mass absorption coefficient (MAC) and single scattering albedo (SSA). We utilized three field missions that were conducted over the SEA ocean between 2016 and 2018. Specifically, we used (1) ground-based measurements from the DOE ARM Mobile Facility (AMF1), which was deployed at Ascension Island (ASI) for the LASIC (Layered Atlantic Smoke Interactions with Clouds) campaign between June 2016 and October 2017, (2) airborne measurements from the UK CLARIFY (Clouds and Aerosol Radiative impacts and Forcing) campaign during Aug-Sep-2017, and (3) airborne measurements from the ORACLES (Observations of Aerosols above Clouds and their interactions) campaign during Aug-2017, and Sep-Oct-2018. The three campaigns cover a relatively large region, from the western African coast on the east towards Ascension Island in the middle of the SEA to the west. We used the data gathered by these campaigns to find how BB properties and composition change from near emission sources (the ORACLES campaign flights) downstream (the CLARIFY flights and the ground based LASIC measurements). We used particle trajectory following methodologies to connect the measurements from the different campaigns, which allowed us to follow a certain aerosol plume (airmass) from near-source towards Ascension Island. We found out that atmospheric aging processes governed by the UV light from the sun (photochemistry) and cloud processes (aqueous chemistry) govern the changes seen in the particle composition during the transport were more dominant in dictating aerosol composition than specific emission composition or source types. We assessed how aerosol optical properties change during the BB season and what are the main drivers of this change. We found that the enhanced ratio of BC to CO is well correlated with single scattering albedo (SSA) and mass absorption coefficient (MACBC), providing a simple way to estimate the aerosol optical characteristics in the south-eastern Atlantic Ocean. From the analysis of the location of BB, the primary source fuel, the water content in the fuel, combined with the mean cloud cover and precipitation in the transport areas of the BB plume, we conclude that the increase in BC/CO from June to August is likely to be caused by burning becoming more flaming (hot fires), and the decrease in BC/CO in September and October may be caused by smoldering (colder) fires. We found that aerosol hygroscopicity increases with decreasing altitude below 2km, and that enhanced BB hygroscopicity at lower altitudes is mainly due to a lower organic aerosol (OA) fraction, increased sulfate fraction, and greater hygroscopicity parameter of OA at lower altitudes.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Aerosol Composition, Mixing State, and Phase State of Free Tropospheric Particles and Their Role in Ice Cloud Formation

The prediction of ice cloud formation in the atmosphere remains challenging. Free tropospheric aerosols can act as ice nucleating particles (INPs), affecting cloud properties and precipitation. The physicochemical properties of free tropospheric particles are modified upon long-range transport by different atmospheric processes. These modifications affect the ice formation potential of individual particles. We investigated free tropospheric particles collected at the remote Pico Mountain Observatory at 2225m a.s.l. in the North Atlantic Ocean using multimodal microspectroscopy and chemical imaging techniques. We probed their ice nucleation activity using an ice nucleation stage interfaced with an environmental scanning electron microscope. Retroplume analysis, chemical imaging, and micro-spectroscopy analysis indicated that the size-resolved chemical composition, mixing state, and phase state of the articles with similar aging times but different transport patterns were substantially different. Relative humidity-dependent glass transition temperatures estimated from meteorological conditions were consistent with the observed organic component of the particles' phase. More viscous (solid and semi-solid-like) particles are more ice active in deposition mode at temperature ranging from 205-220 K than those less viscous particles. Finally, this study provides a better understanding of the phase and mixing state of long range transported free tropospheric aerosols and their role in ice cloud formation.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1999

Quantifying Uncertainties in the Thermo-Mechanical Properties of Particulate Reinforced Composites

The present paper reports results from a computational simulation of probabilistic particulate reinforced composite behavior. The approach consists use of simplified micromechanics of particulate reinforced composites together with a Fast Probability Integration (FPI) technique. Sample results are presented for a Al/SiC(sub p)(silicon carbide particles in aluminum matrix) composite. The probability density functions for composite moduli, thermal expansion coefficient and thermal conductivities along with their sensitivity factors are computed. The effect of different assumed distributions and the effect of reducing scatter in constituent properties on the thermal expansion coefficient are also evaluated. The variations in the constituent properties that directly effect these composite properties are accounted for by assumed probabilistic distributions. The results show that the present technique provides valuable information about the scatter in composite properties and sensitivity factors, which are useful to test or design engineers.

Mital, Subodh K.↗

NASA NTRSDate not supplied

Modeling of Particle Transport and Impact in Transient, Multiphase Oxidizer-Rich Environments Using Computational Fluid Dynamics and Lagrangian Particle Tracking

Particle impacts from foreign object debris (FOD) in an oxidizer-rich environment have been shown to be a credible and significant risk for ignition and failure of components and vehicles. The risk of particle ignition is dependent on many factors, including particle impact velocity/energy and fluid composition (i.e. fluid phase, species presence, and state). Prediction of particle transport and particle impacts in relevant environments, including transient, multiphase flows, is important for assessing the risk and avoiding repeated expensive system level tests. The capability to model both the fluid dynamics and particle transport in complex three-dimensional geometries and multiphase environments has been developed at Marshall Space Flight Center (MSFC) in the propulsion fluid dynamic branch (ER42) by utilizing computational fluid dynamics (CFD) simulations and Lagrangian particle tracking. Using CFD tools, including density-based Loci/CHEM with a cavitation model and pressure-based Loci/STREAM with a volume of fluids model, MSFC/ER42 has provided particle impact predictions to multiple projects for oxidizer compatibility assessments. Simulations of transient, multiphase environments such as liquid slugs flowing through tubing and cavitating flow in valves have been completed alongside one-way coupled Lagrangian particle tracking to predict particle impacts.

M.V. Fischels↗

NASA NTRS1985

Mass spectra of neutral particles released during electrical breakdown of thin polymer films

A special type of time-of-flight mass spectrometer triggered from the breakdown event was developed to study the composition of the neutral particle flux released during the electrical breakdown of polymer films problem. Charge is fed onto a metal-backed polymer surface by a movable smooth platinum contact. A slowly increasing potential from a high-impedance source is applied to the contact until breakdown occurs. The breakdown characteristics is made similar to those produced by an electron beam charging system operating at similar potentials. The apparatus showed that intense instantaneous fluxes of neutral particles are released from the sites of breakdown events. For Teflon FEP films of 50 and 75 microns thickness the material released consists almost entirely of fluorocarbon fragments, some of them having masses greater than 350 atomic mass units amu, while the material released from a 50 micron Kapton film consists mainly of light hydrocarbons with masses at or below 44 amu, with additional carbon monoxide and carbon dioxide. The apparatus is modified to allow electron beam charging of the samples.

Kendall, B. R. F.↗

DOE OSTI2020

Method for producing nanoparticles and the nanoparticles produced therefrom

Disclosed herein is a method comprising disposing a container containing a metal and/or ferromagnetic solid and abrasive particles in a static magnetic field; where the container is surrounded by an induction coil; activating the induction coil with an electrical current, to heat up the metallic or ferromagnetic solid to form a fluid; generating sonic energy to produce acoustic cavitation and abrasion between the abrasive particles and the container; and producing nanoparticles that comprise elements from the container, the metal and/or the ferromagnetic solid and the abrasive particles. Disclosed herein too is a composition comprising first metal or a first ceramic; and particles comprising carbides and/or nitrides dispersed therein. Disclosed herein too is a composition comprising nanoparticles comprising chromium carbide, iron carbide, nickel carbide, γ-Fe and magnesium nickel.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Method for producing nanoparticles and the nanoparticles produced therefrom

Manuel, Michele Viola↗

DOE OSTI2023

Method for producing nanoparticles and the nanoparticles produced therefrom

Manuel, Michele Viola↗

DOE OSTI2023

Method for producing nanoparticles and the nanoparticles produced therefrom

Manuel, Michele Viola↗

NASA NTRS2006

Interplanetary Shocks and "Suprathermal" Flare Particles

We use ion-composition data from ACE/ULEIS, low energy electrons from ACE/EPAM, high energy protons from SoHO/ERNE, radio data from Wind/WAVES, and solar wind data from ACE/SWEPAM and ACE/MAG to investigate the solar and interplanetary circumstances near the times of passage of near-Earth shocks. We are particularly interested in claims that local acceleration by some interplanetary shocks produces Fe/O > 0.3 ('Fe-rich' shocks). The choice of the specific interval used to calculate the Fe/O ratio is extremely important because shock-accelerated particles can be masked by particles from flare events, related or unrelated to the shock, that have Fe/O > 0.3. We conclude that shock- accelerated populations have Fe/0<0.3. We illustrate 5 events which have been reported to be Fe-rich and for which Fe/O increases with energy in the 0.5-2 MeV/nuc range. We find that in each case there are direct flare particles included in the averaging time interval. We also demonstrate that the Fe/O ratio increases as a result of the averaging time interval being too large.

Cane, H. V.↗

NASA NTRS2017

Characterization of Biological Fallout Particles of Cleanrooms to Measure Spacecraft Cleanliness

NASA cleanrooms are humidity, temperature-regulated, and particle contaminant-controlled environments used for spacecraft assembly. Microorganisms, which are crucial contaminants shed from humans and transported through the environment, can adapt to the oligotrophic cleanroom conditions. These biogenic particles need to be identified to extend our knowledge of biological contamination for future NASA mission use. Here, we devised an aluminum coupon with polycarbonate filter setup to collect fallout particles from an ISO 5 and an ISO 7 cleanroom. We demonstrated the presence of microbial particles, as standalone entities and associated with inert particles in cleanroom environments. The contamination was confirmed as biogenic in virtue of estimating the elemental composition of individual and aggregated particles using an epifluorescence and Field Emission Scanning Electron Microscopy (FESEM) coupled with an energy dispersive X-ray analysis (EDX). Epifluorescence microscopy showed that the particles were stained less (25%) with SYTO 9 and more (75%) with propidium iodide, suggesting that the suspected biogenic particles are membrane-compromised. Remarkably, biological particles such as bacteria and fungal spores/hyphae were observed at sizes ranging from 2 to 70 µm, with abundant C and O elemental signatures and essential tracers (Na, Mg, K, Ca and Cl). Inert particles (2 to 500 µm) that were characterized included compositions such as silica (SiO2), aluminosilicates (Al, Si), and carbonaceous fibers. Furthermore, we designed and illustrated a unique correlative epifluorescence and FE-SEM method to strengthen this approach by acquiring the same biogenic particles in the same filter coupon for a one-to-one comparison. Interestingly, the SYTO 9 stained particles showed abundant C and O elemental signature implying that they are viable microbial particles. Constant evaluation of cleanroom biological and inert particles will help to characterize biological contamination for future NASA missions (e.g. Mars 2020).

Malli Mohan, Ganesh Babu↗

NASA NTRS1993

Visible-infrared properties of controlled laboratory soils

Almost all surfaces available for remote observation consist of particulate materials or soils. The distribution of mean particle sizes depend on the original material and physical and chemical processes that have acted on the surface over time. It is well known that the optical and infrared spectral properties of materials depends on the particle size. There has been little detailed study, however, of natural soils, namely particulate materials with a range of particle sizes. Current models for intimate mixing typically use an average particle size in calculations and are most successful when the particle size is constrained by known sieve fractions. Preliminary results of a study in which soils were prepared with a known composition and range of particle sizes are reported. This discussion presents the overall visible to infrared properties of these synthetic soils and evaluates the mid-infrared properties.

Pieters, C. M.↗

DOE OSTI2023

Mesoscale shock structure in particulate composites

Multiscale experiments in heterogeneous materials and the knowledge of their physics under shock compression are limited. Here, this study examines the multiscale shock response of particulate composites comprised of soda-lime glass particles in a PMMA matrix using full-field high speed digital image correlation (DIC) for the first time. Normal plate impact experiments, and complementary numerical simulations, are conducted at stresses ranging from 1.1 - 3.1 GPa to elucidate the mesoscale mechanisms responsible for the distinct shock structure observed in particulate composites. The particle velocity from the macroscopic measurement at continuum scale shows a relatively smooth velocity profile, with shock thickness decreasing with an increase in shock stress, and the composite exhibits strain rate scaling as the second power of the shock stress. In contrast, the mesoscopic response was highly heterogeneous, which led to a rough shock front and the formation of a train of weak shocks traveling at different velocities. Additionally, the normal shock was seen to diffuse the momentum in the transverse direction, affecting the shock rise and the rounding-off observed at the continuum scale measurements. The numerical simulations indicate that the reflections at the interfaces, wave scattering, and interference of these reflected waves are the primary mechanisms for the observed rough shock fronts.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Operando Acoustic Monitoring of SEI Formation and Long-Term Cycling in NMC/SiGr Composite Pouch Cells

Stable long-term cycling and solid-electrolyte-interphase (SEI) formation are key challenges in the design of Si/graphite composites as Li-ion battery (LIB) anode materials. Typically, these long-term cycling properties are examined in flooded half-cell settings making use of a Li-metal counter electrode and a Si/graphite working electrode. This form factor has the advantage of offering an unlimited supply of Li-ions and electrolyte, thus isolating performance degradation to the passivation of the working electrode. However, half-cell studies are ineffective in revealing performance and degradation mechanisms of the Si/graphite composite in a more commercially realistic full cell setting. This paper outlines an operando acoustic technique that can offer insights on SEI formation and capacity degradation of Si/graphite composites in a full cell setting. Through a combination of electrochemical and chemical analyses, we show that increasing passivation of the silicon particles in the Si/graphite composite anode is correlated with an increase in the acoustic time-of-flight shift. We further show that temporary loss of the acoustic signal during the first cycle is associated with significant gassing of the cell. The operando acoustic technique outlined here is low-cost, simple to setup and has the potential for localized resolution, indicating usefulness in commercial-scale Si/graphite cell quality control and diagnosis.

42 ENGINEERING↗

NASA NTRS1986

Galactic cosmic ray composition

An assessment is given of the galactic cosmic ray source (GCRS) elemental composition and its correlation with first ionization potential. The isotopic composition of heavy nuclei; spallation cross sections; energy spectra of primary nuclei; electrons; positrons; local galactic reference abundances; comparison of solar energetic particles and solar coronal compositions; the hydrogen; lead; nitrogen; helium; and germanium deficiency problems; and the excess of elements are among the topics covered.

Meyer, J. P.↗

DOE OSTI2020

Customized Chiral Colloids

This contribution describes a synthetic strategy for the fabrication of multicomponent colloidal “molecules” with controllable complex morphologies and compositionally distinct lobes. Using 3-(trimethoxysilyl)propyl methacry-late (TPM) as the building block, the methodology enables a scalable bulk synthesis of customized chiral colloidal particles with geometric and compositional chirality by sequential seeded growth method. Finally, the synthetic protocol presents a versatile platform for constructing colloidal molecules with multiple components having customized shapes and functionalities, with the potential to impact the design of chromatic patchy particles, colloidal swimmers and chiral optical materials, as well as informing programmable assembly.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

A robust clustering algorithm for analysis of composition-dependent organic aerosol thermal desorption measurements

Abstract. One of the challenges of understanding atmospheric organic aerosol (OA) particles stems from its complex composition. Mass spectrometry is commonly used to characterize the compositional variability of OA. Clustering of a mass spectral dataset helps identify components that exhibit similar behavior or have similar properties, facilitating understanding of sources and processes that govern compositional variability. Here, we developed an algorithm for clustering mass spectra, the noise-sorted scanning clustering (NSSC), appropriate for application to thermal desorption measurements of collected OA particles from the Filter Inlet for Gases and AEROsols coupled to a chemical ionization mass spectrometer (FIGAERO-CIMS). NSSC, which extends the common density-based special clustering of applications with noise (DBSCAN) algorithm, provides a robust, reproducible analysis of the FIGAERO temperature-dependent mass spectral data. The NSSC allows for the determination of thermal profiles for compositionally distinct clusters of mass spectra, increasing the accessibility and enhancing the interpretation of FIGAERO data. Applications of NSSC to several laboratory biogenic secondary organic aerosol (BSOA) systems demonstrate the ability of NSSC to distinguish different types of thermal behaviors for the components comprising the particles along with the relative mass contributions and chemical properties (e.g., average molecular formula) of each mass spectral cluster. For each of the systems examined, more than 80 % of the total mass is clustered into 9–13 mass spectral clusters. Comparison of the average thermograms of the mass spectral clusters between systems indicates some commonality in terms of the thermal properties of different BSOA, although with some system-specific behavior. Application of NSSC to sets of experiments in which one experimental parameter, such as the concentration of NO, is varied demonstrates the potential for mass spectral clustering to elucidate the chemical factors that drive changes in the thermal properties of OA particles. Further quantitative interpretation of the thermograms of the mass spectral clusters will allow for a more comprehensive understanding of the thermochemical properties of OA particles.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Measurement report: Comparison of wintertime individual particles at ground level and above the mixed layer in urban Beijing

Beijing has been suffering from frequent severe air pollution events, with concentrations affected significantly by the mixed-layer height. Major efforts have been made to study the physico-chemical properties, compositions, and sources of aerosol particles at ground level. However, little is known about the morphology, elemental composition, and mixing state of aerosol particles above the mixed layer. In this work, we collected individual aerosol particles simultaneously at ground level (2 m above ground) and above the mixed layer in urban Beijing (within the Atmospheric Pollution and Human Health in a Chinese Megacity, APHH-Beijing, 2016 winter campaign). The particles were analyzed offline by transmission electron microscopy coupled with energy dispersive X-ray spectroscopy. Our results showed that the relative number contribution of mineral particles to all measured particles was much higher during non-haze periods (42.5 %) than haze periods (18.1 %); in contrast, internally mixed particles contributed more during haze periods (21.9 %) than non-haze periods (7.2 %) at ground level. In addition, more mineral particles were found at ground level than above the mixed-layer height. Around 20 % of individual particles showed core–shell structures during haze periods, whereas only a few core–shell particles were observed during non-haze periods (2 %). The results showed that the particles above the mixed layer were more aged, with a larger proportion of organic particles originating from coal combustion. Our results indicate that a large fraction of the airborne particles above the mixed layer come from surrounding areas influenced by coal combustion activities. This source contributes to the surface particle concentrations in Beijing when polluted air is mixed down to the ground level.

54 ENVIRONMENTAL SCIENCES↗