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NASA NTRS2015

Topical Issue on Optical Particle Characterization and Remote Sensing of the Atmosphere: Part II

This represents the second topical issue on optical particle characterization and remote sensing. These two issues resulted from recent interest in increasing our understanding of the Earth-atmosphere system that has been a scientific and political priority for the last few decades. While the initial issue had a stronger focus on microphysics and its implications to the Earth-atmosphere system, this issue is more applied, with a heavier weighting on remote-sensing aspects, atmospheric information retrieval. The first issue was roughly divided into studies that focused on observations of aerosols, associated properties of aerosols and their effects on light-scattering, retrievals of aerosol properties and novel applications.This topical issue is the second of two parts. Within this issue we analyze different aspects of the problem of atmospheric characterization and present a broad overview of the topical area, with a focus especially on lidar measurements and information retrieval. Research includes the development of new observational techniques, theory, experiment and atmospheric characterizations ranging from fundamental microphysical properties of individual aerosol particles to broad characterizations of the entire atmosphere.

remote sensing↗
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↗
NASA NTRS2001

Correlation of Upper-Atmospheric Be-7 With Solar Energetic Particle Events

Surprisingly large concentrations of radioactive Be-7 have been found in the upper atmosphere at levels of one to three orders of magnitude greater than observed in the stratosphere. This phenomenon was originally observed on the LDEF satellite which was recovered in January 1990 following a period of extremely high solar activity in the fall of 1989. We report on follow-up measurements on the Russian COSMOS and RESURS F1 spacecraft during the period of 1996 to 1999 which was a period of minimal to moderate solar activity. The Be-7 concentrations observed on these flights were down substantially from the LDEF observations but were still one to two orders of magnitude higher than stratospheric levels. A significant correlation is observed between the Be-7 activity and the combined fluence of solar energetic protons (SEP) and galactic cosmic-ray (GCR) protons. The Be-7 activity is not correlated with overall solar activity as represented by the solar x-ray flux. We discuss possible mechanisms for the solar proton correlation. However, it is likely that the Be-7 is ionized and it is unknown how this will affect the calculations. There were several large solar flares in the fall of 1989 that produced extraordinarily intense solar particle events at the Earth and record geophysical disturbances. These may have acted to increase production of Be-7 from spallation in the stratosphere and also to enhance transport to higher altitudes from the effects of heating and expansion of the upper atmosphere. Be-7 in the upper atmosphere may also have been produced directly at the Sun. Be-7 and Li-7 are produced in solar flares when accelerated alpha-particles fuse with He-4 in the solar atmosphere. Under optimistic assumptions for Sun to Earth transport and subsequent insertion into low Earth orbit, a Be-7 density of about 10(exp -7) atom/cubic cm at 310 km is estimated.

Phillips, G. W.↗
DOE OSTI2023

Nonequilibrium Behavior in Isoprene Secondary Organic Aerosol

Recent studies have shown that instantaneous gas-particle equilibrium partitioning assumptions fail to predict SOA formation, even at high relative humidity (~85%), and photochemical aging seems to be one driving factor. In this study, we probe the minimum aging time scale required to observe nonequilibrium partitioning of semivolatile organic compounds (SVOCs) between the gas and aerosol phase at ~50% RH. Seed isoprene SOA is generated by photo-oxidation in the presence of effloresced ammonium sulfate seeds at <1 ppbv NO x , aged photochemically or in the dark for 0.3–6 h, and subsequently exposed to fresh isoprene SVOCs. Our results show that the equilibrium partitioning assumption is accurate for fresh isoprene SOA but breaks down after isoprene SOA has been aged for as short as 20 min even in the dark. Modeling results show that a semisolid SOA phase state is necessary to reproduce the observed particle size distribution evolution. The observed nonequilibrium partitioning behavior and inferred semisolid phase state are corroborated by offline mass spectrometric analysis on the bulk aerosol particles showing the formation of organosulfates and oligomers. Here, the unexpected short time scale for the phase transition within isoprene SOA has important implications for the growth of atmospheric ultrafine particles to climate-relevant sizes.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1984

Oxygen isotopes in deep sea spherules

The determination of the genetic relationships between the dust and small particles in the solar system, and the meteorites and larger bodies are examined. Oxygen isotopes proved useful in the identification of such relationships between one meteorite group and another. Of the various samples of submillimeter extraterrestrial particles available for laboratory study, only the deep sea spherules are abundant enough for precise oxygen isotope analysis using existing techniques. Complications arise in interpretation of the isotopic data, since these particles were melted during passage through the Earth's atmosphere, and have been in contact with seawater for prolonged periods. Spherules that were originally silicates are considered with the originally metallic ones to deduce their preterrestrial isotopic compositions. The type 1 spherules which enter the atmosphere as metallic particles, contain only atmospheric oxygen. The type S spherules contain a mixture of atmospheric oxygen and their original extraterrestrial oxygen. It is suggested that the Earth's mesosphere is strongly enriched in heavy isotopes of oxygen at altitudes near 90 km at which the iron particles are oxidized. Fractionation due to the combined diffusion of O atoms and O2 molecules may be responsible.

Mayeda, T. K.↗
DOE OSTI2020

Aerosol Optical Tweezers Elucidate the Chemistry, Acidity, Phase Separations, and Morphology of Atmospheric Microdroplets

Aerosol particles represent unique chemical environments because of their high surface area-to-volume ratio that promotes the effects of interfacial chemistry in confined environments. Properties such as viscosity, diffusivity, water content, pH, and morphology—following liquid–liquid phase separation—can strongly alter how a particle interacts with condensable vapors and reactive trace gases, thus modifying its continual evolution and environmental effects. Our understanding of this chemical evolution of atmospheric particulate matter and its environmental impacts is largely limited by our ability to directly observe how these critical particle properties respond to the addition or reactive uptake of new chemical components. Aerosol optical tweezers (AOT) stably trap particles in focused laser beams, providing positional control and the retrieval of many of these critical properties required to understand and predict the chemistry of aerosolized microdroplets. The analytical power of the AOT stems from the retrieval of the cavity-enhanced Raman spectrum induced by the trapping laser. Analysis of the whispering gallery modes (WGMs) that resonate as a standing wave around the droplet’s interface, provide high accuracy measurements of the droplet’s size, refractive index (and thus a measurement of composition), and can distinguish between core–shell, partially engulfed, and homogeneous morphologies. In this study, we have advanced the ability to determine the properties of the core and shell phases in biphasic droplets, including obtaining high-accuracy pH measurements. These capabilities were applied to perform AOT physical chemistry experiments on authentic secondary organic aerosol (SOA) produced directly in the AOT chamber by ozonolysis of terpene vapors. The propensity of the SOA to phase separate as a shell from a wide range of nonpolar to polar core phases was observed, along with the discovery of a stable emulsified state of SOA particles in an aqueous salt droplet. Micron-thick SOA shells did not impede the gain or loss of water or squalane from the core to the surrounding air, indicating no significant diffusional limitations to condensational growth or partitioning even under dry conditions. These experiments formed the foundation of a new framework that predicts how the phase-separated morphology of complex aerosols containing organic carbon evolves during continual atmospheric oxidation processes. Increases in oxidation state will quickly drive conversion from a partially engulfed to core–shell morphology that has dramatically different chemical reactivity since the core phase is completely concealed by the shell. The recent advances in the experimental capabilities of the AOT technique such as presented here enable novel experimental methodologies that provide insights into the chemistry and multidimensional properties of aerosol microdroplets, and how these coevolve and respond to continual chemical reactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1983

The USRA workshop report: Electrostatic fog dispersal

The Workshop was held at the National Center for Atmospheric Research (NCAR) in Boulder, Colorado, on February 1-2, 1983. The Workshop was attended by seventeen experts in the scientific fields of fog and cloud physics, charged-particle electrodynamics, atmospheric turbulence, atmospheric electricity, and electro-gasdynamics. The major objective of the Workshop was to assess the scientific merits and scientific basis of the proposed system and to assess its potential for operational application.

Davis, M. H.↗
DOE OSTI2023

GeoCarb Calibration Campaign Field Campaign Report

The GeoCarb Calibration Campaign, referred to as the Total Carbon Column Observing Network (TCCON) calibration campaign within this report for clarity, involved a series of single- and multiple-day Bruker EM27/SUN Fourier transform infrared (FTIR) spectrometer deployments at the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility’s Southern Great Plains (SGP) observatory in Oklahoma. The EM27/SUN instruments directly measure infrared solar radiation in a wavelength range from 4000 to 11000 cm -1 at a spectral resolution of 0.5 cm -1 and varied temporal resolution of approximately 15 seconds. The solar radiation observed by these spectrometers contains information about the concentrations of atmospheric constituents present between the instruments and the top of the atmosphere, as every gas and particle in the atmosphere absorbs solar radiation at different wavelengths depending on their physical and chemical makeup. Through retrieval algorithm processing, the solar radiation data collected by EM27/SUN instruments can be used to infer total column dry-air mole fractions, or total column concentrations, of different trace gases present in the atmosphere. These total column concentrations, denoted as Xgas , represent the concentration, in ppb or ppm, of a trace gas in the column of atmosphere between an instrument and the top of the atmosphere. EM27/SUN instruments are primarily used to infer total column concentrations of carbon dioxide (CO 2 ), carbon monoxide (CO), methane (CH 4 ), and water vapor.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1977

Magnetospheric Physics

Dynamic phenomena associated with the plasmasphere, and energy and momentum transferred from the solar wind to the upper atmosphere by means of magnetic field-aligned currents are discussed. Both the LEO and GEO space stations offer potential opportunities to probe the detailed electrical structure of the space plasmas, particle beam atmospheric penetration, beam drifts in the presence of perpendicular electric fields, and permit to study multi-echo dynamics.

Source record↗
DOE OSTI2025

Size-Resolved Chemical Composition of Particles Collected Using STAC at the Ground Site During the SAIL Campaign in Gunnison, Colorado

Aerosol particles were collected using a four-stage Size and Time-resolved Aerosol Collector (STAC) during the SAIL field campaign. Each stage of STAC separates particles into distinct aerodynamic size fractions with 50% cut-off diameters: Stage A: 2.27 µm Stage B: 0.615 µm Stage C: 0.421 µm Stage D: 0.119 µm Each stage provides both size- and time-resolved sampling, enabling investigation of particle composition across different atmospheric regimes. Only a subset of samples was selected for analysis based on prevailing meteorological conditions (e.g., temperature, humidity, and air-mass influence) to capture representative aerosol types under distinct weather patterns. Collected substrates were first examined under Scanning Electron Microscopy (SEM) to evaluate particle loading, morphology, and spatial distribution. Subsequently, Computer-Controlled Scanning Electron Microscopy with Energy-Dispersive X-ray Spectroscopy (CCSEM/EDX) was performed to obtain size-resolved elemental composition of individual particles. A rule-based classification scheme was applied to categorize particles into major compositional groups (e.g., biological, carbonaceous, dust, sulfate, Na-rich, and mixed types). This dataset provides high-resolution morphological and chemical information on atmospheric particles collected during the SAIL campaign, offering insights into the influence of meteorology on aerosol composition and mixing state.

Size and Time-resolved Aerosol Collector↗
NASA NTRS1995

Viking Lander image analysis of Martian atmospheric dust

We have reanalyzed three sets of Viking Lander 1 and 2 (VL1 and VL2) images of the Martian atmosphere to better evaluate the radiative properties of the atmospheric dust particles. The properties of interest are the first two moments of the size distribution, the single-scattering albedo, the dust single-scattering phase function, and the imaginary index of refraction. These properties provide a good definition of the influence that the atmospheric dust has on heating of the atmosphere. Our analysis represents a significant improvement over past analyses (Pollack et al. 1977,1979) by deriving more accurate brightnesses closer to the sun, by carrying out more precise analyses of the data to acquire the quantities of interest, and by using a better representation of scattering by nonspherical particles. The improvements allow us to better define the diffraction peak and hence the size distribution of the particles. For a lognormal particle size distribution, the first two moments of the size distribution, weighted by the geometric cross section, are found. The geometric cross-section weighted mean radius (r(sub eff)) is found to be 1.85 +/- 0.3 microns at VL2 during northern summer when dust loading was low and 1.52 +/- 0.3 microns at VL1 during the first dust storm. In both cases the best cross-section weighted mean variance (nu(eff)) of the size distribution is equal to 0.5 +/- 0.2 microns. The changes in size distribution, and thus radiative properties, do not represent a substantial change in solar energy deposition in the atmosphere over the Pollack et al. (1977,1979) estimates.

Pollack, James B.↗
NASA NTRS1995

Viking Lander image analysis of Martian atmospheric dust

We have reanalyzed three sets of Viking Lander 1 and 2 (VL1 and VL2) images of the Martian atmosphere to better evaluate the radiative properties of the atmospheric dust particles. The properties of interest are the first two moments of the size distribution, the single-scattering albedo, the dust single-scattering phase function, and the imaginary index of refraction. These properties provide a good definition of the influence that the atmospheric dust has on heating of the atmosphere. Our analysis represents a significant improvement over past analyses (Pollack et al. 1977, 1979) by deriving more accurate brightness closer to the sun, by carrying out more precise analyses of the data to acquire the quantities of interest, and by using a better representation of scattering by nonspherical particles. The improvements allow us to better define the diffraction peak and hence the size distribution of the particles. For a lognormal particle size distribution, the first two moments of the size distribution, weighted by the geometric cross section, are found. The geometric cross-section weighted mean radius r(sub eff) is found to be 1.85 +/- 0.3 micrometers at VL2 during northern summer when dust loading was low and 1.52 +/- 0.3 micrometers at VL1 during the first dust storm. In both cases the best cross-section weighted mean variance nu(sub eff) of the size distribution is equal to 0.5 +/- 0.2 micrometers. The changes in size distribution, and thus radiative properties, do not represent a substantial change in solar energy deposition in the atmosphere over the Pollak et al. (1977, 1979) estimates.

Pollack, James B.↗
NASA NTRS1992

Ejecta patterns of Meteor Crater, Arizona derived from the linear un-mixing of TIMS data and laboratory thermal emission spectra

Accurate interpretation of thermal infrared data depends upon the understanding and removal of complicating effects. These effects may include physical mixing of various mineralogies and particle sizes, atmospheric absorption and emission, surficial coatings, geometry effects, and differential surface temperatures. The focus is the examination of the linear spectral mixing of individual mineral or endmember spectra. Linear addition of spectra, for particles larger than the wavelength, allows for a straight-forward method of deconvolving the observed spectra, predicting a volume percent of each endmember. The 'forward analysis' of linear mixing (comparing the spectra of physical mixtures to numerical mixtures) has received much attention. The reverse approach of un-mixing thermal emission spectra was examined with remotely sensed data, but no laboratory verification exists. Understanding of the effects of spectral mixing on high resolution laboratory spectra allows for the extrapolation to lower resolution, and often more complicated, remotely gathered data. Thermal Infrared Multispectral Scanner (TIMS) data for Meteor Crater, Arizona were acquired in Sep. 1987. The spectral un-mixing of these data gives a unique test of the laboratory results. Meteor Crater (1.2 km in diameter and 180 m deep) is located in north-central Arizona, west of Canyon Diablo. The arid environment, paucity of vegetation, and low relief make the region ideal for remote data acquisition. Within the horizontal sedimentary sequence that forms the upper Colorado Plateau, the oldest unit sampled by the impact crater was the Permian Coconino Sandstone. A thin bed of the Toroweap Formation, also of Permian age, conformably overlays the Coconino. Above the Toroweap lies the Permian Kiabab Limestone which, in turn, is covered by a thin veneer of the Moenkopi Formation. The Moenkopi is Triassic in age and has two distinct sub-units in the vicinity of the crater. The lower Wupatki member is a fine-grained sandstone, while the upper Moqui member is a fissile siltstone. Ejecta from these units are preserved as inverted stratigraphy up to 2 crater radii from the rim. The mineralogical contrast between the units, relative lack of post-emplacement erosion and ejecta mixing provide a unique site to apply the un-mixing model. Selection of the aforementioned units as endmembers reveals distinct patterns in the ejecta of the crater.

Ramsey, Michael S.↗
NASA NTRS1990

Tunable diode laser IR spectrometer for in situ measurements of the gas phase composition and particle size distribution of Titan's atmosphere

A new instrument, the Probe Infrared Laser Spectrometer (PIRLS), is described for in situ sensing of the gas composition and particle size distribution of Titan's atmosphere on the NASA/ESA Cassini mission. For gas composition measurements, several narrow-band (0.0001/cm) tunable lead-salt diode lasers operating near 80 K at selected mid-IR wavelengths are directed over a path length defined by a small reflector extending over the edge of the probe spacecraft platform; volume mixing ratios of 10 to the -9th should be measurable for several species of interest. A cloud-particle-size spectrometer using a diode laser source at 780 nm shares the optical path and deployed reflector; a combination of imaging and light scattering techniques is used to determine sizes of haze and cloud particles and their number density as a function of altitude.

Webster, Christopher R.↗