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At least 451 records · Page 25
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Coupled Interfacial and Bulk Kinetics Govern the Timescales of Multiphase Ozonolysis Reactions

Chemical transformations in aerosols impact the lifetime of particle phase species, the fate of atmospheric pollutants, and both climate- and health-relevant aerosol properties. Timescales for multiphase reactions of ozone in atmospheric aqueous phases are governed by coupled kinetic processes between the gas phase, the particle interface, and its bulk, which respond dynamically to reactive consumption of O 3 . However, models of atmospheric aerosol reactivity often do not account for the coupled nature of multiphase processes. Herein, to examine these dynamics, we use new and prior experimental observations of aqueous droplet reaction kinetics, including three systems with a range of surface affinities and ozonolysis rate coefficients ( trans -aconitic acid (C 6 H 6 O 6 ), maleic acid (C 4 H 4 O 4 ), and sodium nitrite (NaNO 2 )). Using literature rate coefficients and thermodynamic properties, we constrain a simple two-compartment stochastic kinetic model which resolves the interface from the particle bulk and represents O 3 partitioning, diffusion, and reaction as a coupled kinetic system. Our kinetic model accurately predicts decay kinetics across all three systems, demonstrating that both the thermodynamic properties of O 3 and the coupled kinetic and diffusion processes are key to making accurate predictions. An enhanced concentration of adsorbed O 3 , compared to gas and bulk phases is rapidly maintained and remains constant even as O 3 is consumed by reaction. Multiphase systems dynamically seek to achieve equilibrium in response to reactive O 3 loss, but this is hampered at solute concentrations relevant to aqueous aerosol by the rate of O 3 arrival in the bulk by diffusion. As a result, bulk-phase O 3 becomes depleted from its Henry's law solubility. This bulk-phase O 3 depletion limits reaction timescales for relatively slow-reacting organic solutes with low interfacial affinity (i.e., trans-aconitic and maleic acids, with k rxn ≈ 10 3 -10 4 M -1 s -1 ), which is in contrast to fast-reacting solutes with higher surface affinity (i.e., nitrite, with k rxn ≈ 10 5 M -1 s -1 ) where surface reactions strongly impact the observed decay kinetics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1981

Stratospheric aerosols

The current state of information on stratospheric aerosols is reviewed. Aerosol properties such as size, size distribution, composition, refractive index, number density, extinction, optical depth, and single scattering albedo are considered and generalized as much as possible to be representative of the global aerosol in times of volcanic and nonvolcanic (background) periods. Data are presented that show the global distribution of stratospheric aerosols as measured by the stratospheric aerosol and gas experiment (SAGE) satellite system for background and volcanic (post-Mount St. Helens) conditions. In addition, lidar and dustsonde data are presented that show the changes in stratospheric aerosol over an 8-year period.

Mccormick, M. P.↗
NASA NTRS2008

A Simple Model for the Cloud Adjacency Effect and the Apparent Bluing of Aerosols Near Clouds

In determining aerosol-cloud interactions, the properties of aerosols must be characterized in the vicinity of clouds. Numerous studies based on satellite observations have reported that aerosol optical depths increase with increasing cloud cover. Part of the increase comes from the humidification and consequent growth of aerosol particles in the moist cloud environment, but part comes from 3D cloud-radiative transfer effects on the retrieved aerosol properties. Often, discerning whether the observed increases in aerosol optical depths are artifacts or real proves difficult. The paper provides a simple model that quantifies the enhanced illumination of cloud-free columns in the vicinity of clouds that are used in the aerosol retrievals. This model is based on the assumption that the enhancement in the cloud-free column radiance comes from enhanced Rayleigh scattering that results from the presence of the nearby clouds. The enhancement in Rayleigh scattering is estimated using a stochastic cloud model to obtain the radiative flux reflected by broken clouds and comparing this flux with that obtained with the molecules in the atmosphere causing extinction, but no scattering.

Marshak, Alexander↗
NASA NTRS2010

Possible Influences of Air Pollution, Dust and Sandstorms on the Indian Monsoon

In Asian monsoon countries, such as China and India, human health and safety problems caused by air pollution are becoming increasingly serious, due to the increased loading of atmospheric pollutants from waste gas emissions and from rising energy demand associated with the rapid pace of industrialization and modernization. Meanwhile, uneven distribution of monsoon rain associated with flash floods or prolonged drought, has caused major loss of human life and damage to crops and.property with devastating societal impacts. Historically, air-pollution and monsoons research are treated as separate problems. However recent studies have suggested that the two problems may be intrinsically linked and need to be studied jointly. Fundamentally, aerosols can affect precipitation through radiative effects cif suspended particles in the atmosphere (direct effect) and/or by interfering and changing: the cloud and precipitation formation processes (indirect effect). Based on their optical properties, aerosols can be classified into two types.: those that absorb solar radiation, and those that do not. Both types of aerosols scatter sunlight and reduce the amount of solar radiation from reaching the Earth's surface, causing it to cool. The surface cooling increases atmospheric stability and reduces convection potential, Absorbing aerosols, however, in addition to cooling the surface, can heat the atmosphere. The heating of the atmosphere may reduce the amount of low clouds by increased evaporation in cloud drops. The heating, however, may induce rising motion, enhance low-level moisture, convergence and, hence, increases rainfall, The latent heating from enhanced rainfall may excite feedback processes in the large-scale circulation, further amplify.the initial response to aerosol heating and producing more rain. Additionally, aerosols can increase the concentration of cloud condensation nuclei (CCN), increase cloud amount and decrease coalescence and collision rates, leading to reduced precipitation. However, in the presence of increasing moist and warm air, the reduced coalescence/collision may lead to supercooled drops at higher altitudes where ice precipitation falls and melts. The latent heat release from freezing aloft and melting below implies greater upward heat transport in polluted clouds and invigorate deep convection. In this way, aerosols may lead to increased local convection. Hence, depending on the ambient large-scale conditions and dynamical feedback processes, aerosols' effect on precipitation can be positive, negative or mixed. In the Asian monsoon and adjacent regions, the aerosol forcing and responses of the water cycle are even more complex, Both direct and indirect effects may take place locally and simultaneously, interacting with each other. in addition to local effects, monsoon rainfall may be affected by aerosols transported from other regions and intensified through large-scale circulation and moisture feedback. Thus, dust transported by the large-scale circulation from the adjacent deserts to northern India may affect rainfall over the Bay of Bengal; sulphate and black carbon front industrial pollution in central, southern China and northern India may affect the rainfall regime over the Korean peninsula and Japan; organic and black carbon front biomass burning from Indo-China may modulate the pre-monsoon rainfall regime over southern China and coastal regions, contributing to variability in differential heating and cooling of the atmosphere and to the land-sea thermal contrast. During the pre-monsoon season and monsoon breaks, it has been suggested that radiative forcing by absorbing aerosols have nearly the same order of magnitude as the forcing due to latent heating from convection and surface fluxes. The magnitude of the total aerosol radiative cooling due to sulphates and soot is of the order of 20-40 W/m2 over the Asian monsoon land region in the pre-monsoon season, compared to about 1-2 W/m2 for global warng. However, the combined forcing at the surface and in the atmosphere, including all species. if aerosols, and details of aerosol mixing, and impacts on the energy and water cycles in the monsoon land regions, are not well known.

Lau, William K. M.↗
NASA NTRS2020

Dust Aerosol Retrieval Over the Oceans With the MODIS/VIIRS Dark Target Algorithm: 2. Nonspherical Dust Model

The Dark‐target (DT) aerosol algorithm retrieves spectral Aerosol Optical Depth (AOD) and other aerosol properties from Moderate‐resolution Imaging Spectrometer (MODIS) reflectance observations. Over the ocean, the DT algorithm is known to contain scattering‐angle‐dependent biases in its retrievals of AOD, Angstrom Exponent (AE), and Fine Mode Fraction (FMF) for dust aerosols. Following a two‐step strategy to improve the DT retrieval of dust over ocean, for which the first step is to identify dusty pixels (reported in “Part 1”), in this “Part 2,” we report on construction of a new dust model lookup table (LUT) and the strategy for applying it within the existing DT algorithm. In particular, we evaluate different characterizations of dust optical properties from a variety of frameworks and databases, and compare them with the current DT retrieval assumptions. Substituting the standard operational LUT with a spheroid dust model with identified dusty pixels shows significant improvement when compared with collocated AERONET‐identified dusty pixels. Specifically, the application of the new dust model to dusty pixels reduces their AOD bias from 0.06 to 0.02 while improving the fraction of retrievals within expected error from 64% to 82%. At the same time, the overall bias in AE is reduced from 0.13 to 0.06, and the scattering‐angle‐dependent AE bias is largely eliminated. In testing on two full months of data (April and July), the new retrieval will reduce the monthly mean AOD by up to 0.1 and 0.2 in the north Atlantic and Arabian seas, respectively. The average AE and FMF are also reduced in these dust heavy regions

dust aerosol retrieval↗
NASA NTRS2015

Photopolarimetric Retrievals of Snow Properties

Polarimetric observations of snow surfaces, obtained in the 410-2264 nm range with the Research Scanning Polarimeter onboard the NASA ER-2 high-altitude aircraft, are analyzed and presented. These novel measurements are of interest to the remote sensing community because the overwhelming brightness of snow plagues aerosol and cloud retrievals based on airborne and spaceborne total reflection measurements. The spectral signatures of the polarized reflectance of snow are therefore worthwhile investigating in order to provide guidance for the adaptation of algorithms currently employed for the retrieval of aerosol properties over soil and vegetated surfaces. At the same time, the increased information content of polarimetric measurements allows for a meaningful characterization of the snow medium. In our case, the grains are modeled as hexagonal prisms of variable aspect ratios and microscale roughness, yielding retrievals of the grains' scattering asymmetry parameter, shape and size. The results agree with our previous findings based on a more limited data set, with the majority of retrievals leading to moderately rough crystals of extreme aspect ratios, for each scene corresponding to a single value of the asymmetry parameter.

aspect ratio↗
NASA NTRS1989

Aerosol backscatter studies supporting LAWS

Optimized Royal Signals and Radar Establishment (RSRE), Laser True Airspeed System (LATAS) algorithm for low backscatter conditions was developed. The algorithm converts backscatter intensity measurements from focused continuous-wave (CW) airborne Doppler lidar into backscatter coefficients. The performance of optimized algorithm under marginal backscatter signal conditions was evaluated. The 10.6 micron CO2 aerosol backscatter climatologies were statistically analyzed. Climatologies reveal clean background aerosol mode near 10(exp -10)/kg/sq m/sr (mixing ratio units) through middle and upper troposhere, convective mode associated with planetary boundary layer convective activity, and stratospheric mode associated with volcanically-generated aerosols. Properties of clean background mode are critical to design and simulation studies of Laser Atmospheric Wind Sounder (LAWS), a MSFC facility Instrument on the Earth Observing System (Eos). Previous intercomparisons suggested correlation between aerosol backscatter at CO2 wavelength and water vapor. Field measurements of backscatter profiles with MSFC ground-based Doppler lidar system (GBDLS) were initiated in late FY-88 to coincide with independent program of local rawinsonde releases and overflights by Multi-spectral Atmospheric Mapping Sensor (MAMS), a multi-channel infrared radiometer capable of measuring horizontal and vertical moisture distributions. Design and performance simulation studies for LAWS would benefit from the existence of a relationship between backscatter and water vapor.

Rothermel, Jeffry↗
NASA NTRS1996

The 1996 Subsonic Aircraft: Contrail and Cloud Effects Special Study

During April 1996 NASA, in conjunction with the DOE, will sponsor a multi-aircraft field campaign to better understand the microphysical and radiative properties of cirrus clouds, the origins of ice nuclei and cloud condensation nuclei in the upper troposphere, and the possible role that the commercial subsonic aircraft fleet might play in altering cloud or aerosol properties. The NASA ER-2 aircraft will be used as a remote sensing platform, while the NASA DC-8 aircraft will be used as an in situ measurement platform. In situ observations will include a full set of size distribution measurements from nano-meter to millimeter sizes, ice water content measurements, gas phase and condensed phase chemical measurements, ice crystal optical phase function measurements, lidar observations of cloud top and cloud base, and atmospheric state measurement. The ER-2 will have lidar, microwave ice water path measurements, as well as visible and infrared spectral measurement. In this presentation the highlights of the mission will be presented. The goal will be to address fundamental questions such as the mode of nucleation of cirrus clouds, the composition of the nuclei on which cirrus form, the degree to which aircraft impact cirrus cloud properties.

Toon, Owen B.↗
NASA NTRS2013

Application of Spectral Analysis Techniques in the Intercomparison of Aerosol Data: 1. an EOF Approach to the Spatial-Temporal Variability of Aerosol Optical Depth Using Multiple Remote Sensing Data Sets

Many remote sensing techniques and passive sensors have been developed to measure global aerosol properties. While instantaneous comparisons between pixel-level data often reveal quantitative differences, here we use Empirical Orthogonal Function (EOF) analysis, also known as Principal Component Analysis, to demonstrate that satellite-derived aerosol optical depth (AOD) data sets exhibit essentially the same spatial and temporal variability and are thus suitable for large-scale studies. Analysis results show that the first four EOF modes of AOD account for the bulk of the variance and agree well across the four data sets used in this study (i.e., Aqua MODIS, Terra MODIS, MISR, and SeaWiFS). Only SeaWiFS data over land have slightly different EOF patterns. Globally, the first two EOF modes show annual cycles and are mainly related to Sahara dust in the northern hemisphere and biomass burning in the southern hemisphere, respectively. After removing the mean seasonal cycle from the data, major aerosol sources, including biomass burning in South America and dust in West Africa, are revealed in the dominant modes due to the different interannual variability of aerosol emissions. The enhancement of biomass burning associated with El Niño over Indonesia and central South America is also captured with the EOF technique.

variability↗
NASA NTRS1989

Aerosol analysis with the Coastal Zone Color Scanner - A simple method for including multiple scattering effects

A method for studying aerosols over the ocean using Nimbus-7 CZCS data is proposed which circumvents having to perform radiative transfer computations involving the aerosol properties. The method is applied to the CZCS band 4 at 670 nm, and yields the total radiance (L sub t) backscattered from the top of a stratified atmosphere containing both stratospheric and tropospheric aerosols and the the Rayleigh scattered radiance (L sub r). The radiance which the aerosol would produce in the single scattering approximation is retrieved from (L sub t) - (L sub r) with an error of not greater than 5-7 percent.

Gordon, Howard R.↗
NASA NTRS2011

Validating and Improving Long-Term Aerosol Data Records from SeaWiFS

Natural and anthropogenic aerosols influence the radiative balance of the Earth through direct and indirect interactions with incoming solar radiation. However, the quantification of these interactions and their ultimate effect on the Earth's climate still have large uncertainties. This is partly due to the limitations of current satellite data records which include short satellite lifetimes, retrieval algorithm uncertainty, or insufficient calibration accuracy. We have taken the first steps in overcoming this hurdle with the production and public release of an aerosol data record using the radiances from the Sea-viewing Wide Field-of-View Sensor (Sea WiFS). Sea WiFS was launched in late 1997 and provided exceptionally well-calibrated top-of-atmosphere radiance data until December 2010, more than 13 years. We have partnered this data with an expanded Deep Blue aerosol retrieval algorithm. In accordance with Deep Blue's original focus, the latest algorithm retrieves aerosol properties not only over bright desert surfaces, but also over oceans and vegetated surfaces. With this combination of a long time series and global algorithm, we can finally identify the changing patterns of regional aerosol loading and provide insight into longterm variability and trends of aerosols on regional and global scales. In this work, we provide an introduction to Sea WiFS, the current algorithms, and our aerosol data records. We have validated the data over land and ocean with ground measurements from the Aerosol Robotic Network (AERONET) and compared them with other satellites such as MODIS and MISR. Looking ahead to the next data release, we will also provide details on the implemented and planned algorithm improvements, and subsequent validation results.

Bettenhausen, Corey↗
DOE OSTI2022

Polar Aerosol Vertical Structures and Characteristics Observed with a High Spectral Resolution Lidar at the ARM NSA Observatory

Aerosol vertical distributions impact both the direct and indirect radiative effects of aerosols. High Spectra Resolution Lidar (HSRL) separates between atmospheric molecular signals and aerosol particle signals and therefore can provide reliable measurements of aerosol properties. Six years of HSRL measurements between 2014 and 2019 from the Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) North Slope of Alaska (NSA) atmospheric observatory at Utqiaqvik are used to statistically analyze Arctic aerosol vertical distributions. The annual cycle of aerosol vertical distributions in terms of aerosol particulate backscatter coefficient ($β_p$), lidar scattering ratio (SR), and aerosol particulate depolarization ratio ($δ_p$) profiles at the wavelength of 532 nm shows that Arctic Haze events are prevalent in later winter and spring at the NSA site. Mineral dust is frequently presented in strong aerosol layers in the spring, fall, and winter seasons. Over the summer season, the NSA site has large aerosol loadings that are dominated by small spherical aerosol particles.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Evaluation of a quasi-steady-state approximation of the cloud droplet growth equation (QDGE) scheme for aerosol activation in global models using multiple aircraft data over both continental and marine environments

This research introduces a numerically efficient aerosol activation scheme and evaluates it by using stratus and stratocumulus cloud data sampled during multiple aircraft campaigns in Canada, Chile, Brazil, and China. The scheme employs a quasi-steady-state approximation of the cloud droplet growth equation (QDGE) to efficiently simulate aerosol activation, the vertical profile of supersaturation, and the activated cloud droplet number concentration (CDNC) near the cloud base. The calculated maximum supersaturation values using the QDGE scheme were compared with multiple parcel model simulations under various aerosol and environmental conditions. The differences are all below 0.18 %, indicating good performance and accuracy of the QDGE scheme. We evaluated the QDGE scheme by specifying observed environmental thermodynamic variables and aerosol information from 31 cloud cases as input and comparing the simulated CDNC with cloud observations. The average of mean relative error ($\overline{MRE}$) of the simulated CDNC for cloud cases in each campaign ranges from 17.30 % in Brazil to 25.90 % in China, indicating that the QDGE scheme successfully reproduces observed variations in CDNC over a wide range of different meteorological conditions and aerosol regimes. Additionally, we carried out an error analysis by calculating the maximum information coefficient (MIC) between the MRE and input variables for the individual campaigns and all cloud cases. MIC values were then sorted by aerosol properties, pollution level, environmental humidity, and dynamic condition according to their relative importance to MRE. Based on the error analysis, we found that the magnitude of MRE is more relevant to the specification of input aerosol pollution level in marine regions and aerosol hygroscopicity in continental regions than to other variables in the simulation.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2026

Employing Machine Learning for New Particle Formation Identification and Mechanistic Analysis: Insights From a Six‐Year Observational Study in the Southern Great Plains

We present a supervised machine learning (ML) framework to automatically identify new particle formation (NPF) events and analyze key atmospheric factors associated with their occurrence and growth. We applied ML to detect NPF events using start time and particle concentrations across size ranges, while identifying atmospheric variables including ambient temperature, relative humidity, solar radiation intensity (SRI), wind speed, wind direction, boundary layer height, total organics, sulfate, nitrate, total surface area concentration, sulfur dioxide, and turbulent kinetic energy (TKE). We analyzed a 6-year data set from the Atmospheric Radiation Measurement at the Southern Great Plains (SGP) site in Oklahoma, USA. Using long-term ground-based measurements, we identified NPF events and applied Random Forest Classifiers, which achieved 90%–95% prediction accuracy. Feature importance analysis highlighted SRI, relative humidity, and ambient temperature as the most influential variables, contributing normalized importances of 28%, 17%, and 10%. Partial Dependence Plots (PDPs) indicated that higher SRI and lower relative humidity were critical in promoting NPF formation at SGP. Seasonally, NPF events were more frequent in winter (42.1%) and spring (35.5%), and least in summer (4.0%). Particle growth rates also exhibited a seasonal variation, with the lowest in winter (below 2 nm hr −1 ) and highest in late spring and early summer (exceeding 5 nm hr −1 ). Temperature, turbulent kinetic energy, and aerosol properties were the primary factors of growth rate variability. This study advances predictive modeling of NPF, offers insights for future campaign deployments, and demonstrates the effectiveness of ML in understanding the formation and growth of atmospheric aerosols.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2003

MISR Multi-Angle Imaging SpectroRadiometer

This viewgraph presentation reviews the concept of the Multi-Angle Imaging SpectroRadiometer (MISR), a methodology to use the MISR to retrieve aerosols over water and land. The presentation shows some of the results of the use of the MISR in graphs and charts. Multi-angle remote sensing provides unique ways of retrieving aerosol properties over many surface types, including bright deserts which are major source regions.

global maps↗
NASA NTRS2011

A Pure Marine Aerosol Model, for Use in Remote Sensing Applications

Retrievals of aerosol optical depth (AOD) and related parameters from satellite measurements typically involve prescribed models of aerosol size and composition, and are therefore dependent on how well these models are able to represent the radiative behaviour of real aerosols, This study uses aerosol volume size distributions retrieved from Sun-photometer measurements at 11 Aerosol Robotic Network (AERONET) island sites, spread throughout the world's oceans, as a basis to define such a model for unpolluted maritime aerosols. Size distributions are observed to be bimodal and approximately lognormal, although the coarse mode is skewed with a long tail on the low-radius end, The relationship of AOD and size distribution parameters to meteorological conditions is also examined, As wind speed increases, so do coarse-mode volume and radius, The AOD and Angstrom exponent (alpha) show linear relationships with wind speed, although there is considerable scatter in all these relationships, limiting their predictive power. Links between aerosol properties and near-surface relative humidity, columnar water vapor, and sea surface temperature are also explored. A recommended bimodal maritime model, which is able to reconstruct the AERONET AOD with accuracy of order 0.01-0.02, is presented for use in aerosol remote sensing applications. This accuracy holds at most sites and for wavelengths between 340 nm and 1020 nm. Calculated lidar ratios are also provided, and differ significantly from those currently used in Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) processing.

Sayer, A. M.↗
DOE OSTI2022

Constraining Physical Understanding of Aerosol Loading, Biogeochemistry, and Snowmelt Hydrology from Hillslope to Watershed Scale in the East River Scientific Focus Area

The mountain snowpack is a critical component of regional hydrology, ecology, biogeochemistry, and climate in the Western US. This project leveraged the East River Scientific Focus Area (SFA), as an outdoor laboratory to address a significant gap in our understanding of the mountain snowpack; namely, how atmospheric constituent deposition on snowpack influences snow energy balance and nutrient/chemical cycling, and how snowmelt timing and intensity exerts controls on emergent biogeochemical and ecohydrologic behavior. This aligned with East River SFA goals to integrate landscape scale measurements and physical based modeling tools to improve understanding of controls on runoff production, ecohydrology, biogeochemical cycling, and land surface energy partitioning in high mountain watersheds. The project included observations of snowpack at multiple scales, measurements of snow and deposited aerosols properties, in situ time series of surface energy balance, and spatially distributed, process-based snowmelt modeling.

54 ENVIRONMENTAL SCIENCES↗