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All sourcesNASA NTRSDOE OSTI
NASA NTRS2011

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.↗
DOE OSTI2020

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↗
DOE OSTI2020

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↗
DOE OSTI2024

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↗
NASA NTRS2002

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.↗
DOE OSTI2024

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↗
NASA NTRS2002

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↗
NASA NTRS1984

Structural characterizaiton and gas reactions of small metal particles by high-resolution, in-situ TEM and TED

The existing in-situ transmission electron microscopy (TEM) facility was improved by adding a separately pumped mini-specimen chamber. The chamber contains wire-evaporation sources for three metals and a specimen heater for moderate substrate temperatures. A sample introduction device was constructed, installed, and tested, facilitating rapid introduction of a specimen into the mini-chamber while maintaining the background pressure in that chamber in the 10(-9) millibar range. Small particles and clusters of Pd, grown by deposition from the vapor phase in an in-situ TEM facility on amorphous and crystalline support films of alumina and on ultra-thin carbon films, were analyzed by conventional high-resolution TEM and image analysis in terms of detectability, number density, and size distribution. The smallest particles that could be detected and counted contained no more than 6 atoms; size determinations could be made for particles 1 nm in diameter. The influence of various oxygen plasma treatments, annealing treatments, and of increasing the substrate temperature during deposition was investigated. The TEM technique was employed to demonstrate that under otherwise identica l conditions the lattice parameter of Pd particles in the 1 to 2 nm size range and supported in random orientation on ex-situ prepared mica films is expanded by some 3% when compared to 5 nm size particles. It is believed that this expansion is neither a small-particle diffraction effect nor due to pseudomorphism, but that it is due to a annealing-induced transformation of the small as-deposited particles with predominantly composite crystal structures into larger particles with true f.c.c. structure and thus inherently smaller lattice parameter.

Source record↗
DOE OSTI2017

Experimental strategies for imaging bioparticles with femtosecond hard X-ray pulses

This study explores the capabilities of the Coherent X-ray Imaging Instrument at the Linac Coherent Light Source to image small biological samples. The weak signal from small samples puts a significant demand on the experiment. Aerosolized Omono River virus particles of ~40 nm in diameter were injected into the submicrometre X-ray focus at a reduced pressure. Diffraction patterns were recorded on two area detectors. The statistical nature of the measurements from many individual particles provided information about the intensity profile of the X-ray beam, phase variations in the wavefront and the size distribution of the injected particles. The results point to a wider than expected size distribution (from ~35 to ~300 nm in diameter). This is likely to be owing to nonvolatile contaminants from larger droplets during aerosolization and droplet evaporation. The results suggest that the concentration of nonvolatile contaminants and the ratio between the volumes of the initial droplet and the sample particles is critical in such studies. The maximum beam intensity in the focus was found to be 1.9 × 10 12 photons per µm 2 per pulse. The full-width of the focus at half-maximum was estimated to be 500 nm (assuming 20% beamline transmission), and this width is larger than expected. Under these conditions, the diffraction signal from a sample-sized particle remained above the average background to a resolution of 4.25 nm. Finally, the results suggest that reducing the size of the initial droplets during aerosolization is necessary to bring small particles into the scope of detailed structural studies with X-ray lasers.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2024

High-accuracy method for modeling nucleation and growth of particles

State-of-the-art numerical models describing the kinetics of aerosol particle nucleation and growth from a cooling vapor primarily use a nodal method, in which particles that are smaller than the critical size are omitted from consideration because they are thermodynamically unfavorable. This omission is based on the assumption that most newly formed particles are above the critical size, so that subcritical-size particles are not important to take into account. Due to the nature of the nodal method, it suffers from numerical diffusion, which can cause an artificial broadening of the cluster size distribution leading to a significant overestimation of the number of large-size particles. To address these issues, we propose a more accurate numerical method that explicitly models particles of all sizes, and uses a special numerical scheme that substantially reduces the numerical diffusion and provides high solution accuracy and numerical stability. We extensively compare this novel method to the commonly used nodal solver of the general dynamic equation (GDE) for particle growth and demonstrate that it offers GDE solutions with higher accuracy with low numerical diffusion. Incorporating small subcritical clusters into the solution is crucial for: 1) more precise determination of the entire particle size distribution function and 2) wider applicability of the model to experimental studies with non-monotonic temperature variations leading to particle evaporation. The computational code implementing this numerical method in Python is available upon request.

42 ENGINEERING↗
DOE OSTI2021

Computational fluid dynamics modeling and analysis of silica nanoparticle synthesis in a flame spray pyrolysis reactor

Flame Spray Pyrolysis (FSP) is a method for large-scale production of nanoparticles and nanoscale powders employed in a wide range of industrial applications. Particle size and morphology are complex functions of the physicochemical phenomena occurring in the FSP reactor. An extensive study of FSP-related phenomena can be utilized to develop effective strategies for achieving desired particle size/morphology and scaling up the overall yield of an FSP system. In this work, a computational fluid dynamics (CFD) model of an FSP reactor is developed to simulate the coupling of key phenomena involved in the particle synthesis process: liquid spray breakup and evaporation, mixing, combustion, and particle formation/growth of silica nanoparticles. Herein, the particle sizes and their distributions from the CFD simulations are validated against experimental data. Subsequently, the simulations are utilized to investigate the impact of process parameters on the resultant flame dynamics and particle growth. Firstly, the CFD results show that the particle sizes are strongly correlated with the precursor concentration in the solvent. At lower precursor concentrations, the spread of the distribution is relatively insensitive to the value of the concentration. At higher concentrations, the spread is higher as the collision probability between particles is higher. Secondly, increasing the pilot flow rate increases the length of the pilot flames impacting the local ignition location of the spray flame. Lastly, it is shown that the dispersion gas flow rate strongly influences the spray flame shape. This shape can be used for control of particle growth as it helps determine the regions of high temperature and the residence time of the particles in the high temperature region enabling the design and process optimization of the FSP reactor.

42 ENGINEERING↗
DOE OSTI2014

Modeling kinetic partitioning of secondary organic aerosol and size distribution dynamics: representing effects of volatility, phase state, and particle-phase reaction

Evidence is mounting that the majority of the climatically active aerosols are produced through the growth of smaller particles via secondary organic aerosol (SOA) formation from gas-to-particle conversion of anthropogenic and biogenic volatile organic compounds (VOCs). The timescale of SOA partitioning and the associated size distribution dynamics are expected to depend on the gas-phase oxidation of the precursor VOCs and their products, volatility of these organic solutes, composition and phase state of the pre-existing particles, and diffusivity and reactivity of the solute within the particle phase. This paper describes a new framework for modeling kinetic gas-particle partitioning of SOA, with an analytical treatment for the diffusion-reaction process within the particle phase. The formulation is amenable for eventual use in regional and global climate models, although it currently awaits implementation of the actual particle-phase reactions that are important for SOA formation. In the present work, the model is applied to investigate the competitive growth dynamics of the Aitken and accumulation mode particles while the Kelvin effect and coagulation are neglected for simplicity. The timescale of SOA partitioning and evolution of number and composition size distributions are evaluated for a range of solute volatilities (C*), particle-phase bulk diffusivities (Db), and particle-phase reactivity, as exemplified by a pseudo-first-order rate constant (kc). Results show that irreversible condensation of non-volatile organic vapors (equivalent to ) produces significant narrowing of the size distribution. At the other extreme, non-reactive partitioning of semi-volatile organic vapors is volume-controlled in which the final (equilibrium) size distribution simply shifts to the right on the diameter axis while its shape remains unchanged. However, appreciable narrowing of the size distribution may occur when the pre-existing particles are highly viscous semi-solids such that small particles reach quasi-equilibrium much faster than the large ones. In the case of reactive partitioning (finite ), the size distribution experiences permanent narrowing, which is especially pronounced for Db < 10-13 cm2 s-1 and kc > 0.01 s-1. As a result, both number and composition size distributions are needed to effectively constrain and evaluate the next generation of SOA models that treat phase state thermodynamics, particle-phase diffusion and particle-phase chemical reactions.

Zaveri, Rahul A.↗
DOE OSTI2015

The Influence of Constitutional Supercooling on the Distribution of Te-particles in Melt-Grown CZT

A section of a vertical gradient freeze Cd 0.9 Zn 0.1 Te boule approximately 2100-mm 3 with a planar area of 300-mm 2 was prepared and examined using transmitted IR microscopy at various magnifications to determine the three-dimensional spatial and size distributions of Te-particles over large longitudinal and radial length scales. Te-particle density distributions were determined as a function of longitudinal and radial positions in these strips and exhibited a multi-modal lognormal size density distribution that indicated a slight preference for increasing size with longitudinal growth time, while showing a pronounced cellular network structure. Higher magnification images revealed a typical Rayleigh-instability pearl string morphology with large and small satellite droplets. This study includes solidification experiments in small crucibles of 30:70 mixtures of Cd:Te performed over a wide range of cooling rates that clearly demonstrated a growth instability with Te-particle capture that is suggested to be responsible for one of the peaks in the size distribution using size discrimination visualization. The results are discussed with regard to a manifold Te-particle genesis history as Te-particle direct capture from melt-solid growth instabilities due to constitutional supercooling and as Te-particle formation from the breakup of Te-ribbons via a Rayleigh-Plateau instability.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2016

Low laser power micro-Raman study of Co{sub (1−x)}Mn{sub (x)}Fe{sub 2}O{sub 4} prepared by flash combustion method

Manganese substituted Cobalt ferrites of composition with nominal formula Co{sub (1−x)}Mn{sub (x)}Fe{sub 2}O{sub 4} (x = 0.0, 0.2, 0.4, 0.6, 0.8, 1.0) prepared by the Flash Combustion Method(FCM). The single phase spinel formation of nano ferrites was confirmed by X-ray diffraction techniques and micro - Raman spectroscopy. The particle size calculated from the Scherrer formula varied within 13 to 17 nm. Lattice parameter, nano particle size, and cation distribution were quantified as a function of the Mn-content in the range x = 0.0 to 1.0. Micro-Raman spectroscopic studies yielded convincing evidence for a transformation of the structure.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRSDate not supplied

The Relationship Of Size Distributions To Spectral (300 - 700 Nm) Extinction Parameterization Of Ambient In Situ Aerosols Measured During FIREX-AQ And The Influence Of Aerosol Composition

Hyperspectral (300 - 700 nm, 0.7 nm resolution) aerosol extinction spectra were measured at seven fires in six states in the western United States during the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) field campaign in July and August 2019. Obtained using an in situ aerosol sampling method, these spectra are directly comparable to other in situ aerosol measurements such as size distribution and composition. A previous deployment of the in situ Spectral Aerosol Extinction (SpEx) instrument that measured fine mode aerosols (50% size cut of 1.3 µm particle diameter) around the Korean peninsula showed that over this spectral range 2nd order polynomials provided a better fit to the logarithmically transformed spectra than linear fits (representative of Ångström exponents). The two fit parameters (a1, a2) of the polynomials are related to the classic Ångström exponent but provide additional information via their two-dimensional parameter space. The previous work was limited by the lack of commensurate size distribution information. Here, using the FIREX-AQ spectra set it is possible to expand on the previous analysis in three specific ways: 1) size distribution information is available to further elucidate how size distribution maps into (a1, a2) space, 2) the sampled size distributions include larger particles than the Korean study, and 3) the FIREX-AQ data set exhibits smoke-related spectral features in the UV part of the spectrum that are not present in background air nor were they observed previously in the Korean study. The UV spectral features are particularly intriguing as they likely arise from the absorption component of the extinction measurement and therefore may be related to composition. The relationships between the ambient in situ aerosol size distributions, the extinction spectra, and composition will be presented.

Carolyn Jordan↗
DOE OSTI2021

Developing and Testing a Novel Stochastic Ice Microphysics Parameterization for Cloud and Climate Models Using ARM Field Campaign Data (Final Progress Report)

The major goals of this project were: 1) to use field campaign measurements from DOE’s Atmospheric Radiation Measurement (ARM) program to characterize variability of important parameters describing properties of ice particles in the atmosphere; 2) based on this observational analysis, to develop a parameterization scheme for weather and climate models that stochastically varies these parameters, and implement the new scheme into a weather model called the Weather Research and Forecasting model (WRF); 3) to use WRF coupled with the new stochastic scheme to simulate ARM field campaign thunderstorm cases and analyze how accounting for this parameter variability affects the model simulations. This work was performed jointly between the National Center for Atmospheric Research, University of Oklahoma, and University of Utah. To accomplish these goals, we extended an approach previously developed to characterize the variability in the size distribution of ice particles to parameters that are explicitly represented in models (i.e., relationships between ice particle mass and size, and between particle fall velocity and size). Our project was, to our knowledge, the first to apply observationally-constrained estimates of this parameter variability describing mass-size and fall velocity-size in a modeling framework. Our results showed efficacy of the approach, evaluated using ARM observations. Similarly, to our knowledge, work in this project was the first to propose and evaluate in detail a stochastic approach for unresolved turbulent mixing in high-resolution model simulations against detailed, benchmark large eddy simulations and ARM observations. Results showed some promising behavior, particularly with increased mixing and dilution of air in thunderstorm cores with surrounding environmental air, bringing the stochastic simulations closer to the benchmark large eddy simulations; however, results were somewhat degraded using stochastic mixing compared to observations from the AMIE/DYNAMO field campaign. This project also further refined and applied a modeling methodology called “piggybacking” that can robustly separate dynamical and thermodynamic impacts of model changes, and comparison studies of different models based on cases developed from ARM observations. Finally, this project directly supported three graduate students who completed their PhDs as well as a postdoctoral research fellow.

54 ENVIRONMENTAL SCIENCES↗