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At least 37 records · Page 2

Numerical simulation of advection fog formation on multi-disperse aerosols due to combustion-related pollutants

The effects of multi-disperse distribution of the aerosol population are presented. Single component and multi-component aerosol species on the condensation/nucleation processes which affect the reduction in visibility are described. The aerosol population with a high particle concentration provided more favorable conditions for the formation of a denser fog than the aerosol population with a greater particle size distribution when the value of the mass concentration of the aerosols was kept constant. The results were used as numerical predictions of fog formation. Two dimensional observations in horizontal and vertical coordinates, together with time-dependent measurements were needed as initial values for the following physical parameters: (1)wind profiles; (2) temperature profiles; (3) humidity profiles; (4) mass concentration of aerosol particles; (5) particle size distribution of aerosols; and (6) chemical composition of aerosols. Formation and dissipation of advection fog, thus, can be forecasted numerically by introducing initial values obtained from the observations.

Hung, R. J.↗

Measurements

To interpret the effects of aerosols and gases on the atmosphere, information on the vertical and horizontal distribution of aerosol particles, their size distributions and concentration of precursor gases is required. Measurements of aerosols and gases at frequent intervals and over vast areas of atmosphere generally involve remote sensing techniques. These techniques depend on the optical properties of the species studied. Optical properties can vary greatly with aerosol size and refractive index. Remote sensing instruments look at light scattering, extinction, depolarization, and reflection. The chemical composition, phase equilibria, surface properties, and photochemical behavior of stratospheric aerosols are not clearly understood or adequately measured by current technologies. Areas are listed which need technology development.

Source record↗

Concentrations and size distributions of Antarctic stratospheric aerosols

Particle Measuring Systems laser particle spectrometer (ASAS-X and FSSP) probes were used to measure aerosol particle concentrations and size distributions during 11 ER-2 flights between Punta Arenas (53 deg S) and Antarctica (up to 72 deg S) from August 17 to September 22, 1987. The time resolution was 10 s, corresponding to a spatial resolution of 2 km. The data were divided into two size classes (0.05-0.25 and 0.53-5.5 micron radius) to separate the small particle from the coarse particle populations. Results show that the small-particle concentrations are typical for a background aerosol during volcanic quiescence. This concentration is generally constant along a flight track; in only one instance a depletion of small particles during a polar stratospheric cloud (PSC) encounter was measured, suggesting a nucleation of type I PSC particles on background aerosols. Temporary increases of the coarse particle concentrations indicated the presence of tenuous polar stratospheric clouds that were encountered most frequently at the southernmost portion of a flight track and when the aircraft descended to lower altitudes. During 'particle events', particle modes were found at 0.6-micron radius, corresponding to type I PSCs, and occasionally, at 2.0-micron radius corresponding to type II PSCs.

Ferry, G. V.↗

A Stokes' velocity photographic method for measuring the size distribution of aerosols

Aerosol particles are allowed to settle in a vertical glass walled vessel, and their settling velocity is determined by photographing them while the light entering the camera is being chopped at a known rate. The settling velocity of each particle can be determined from the photographs, and by applying the Stokes' law, one can calculate the radius of each particle. The Stokes' law for a sphere settling freely in a quiet medium is given. If the volume of the photographed region of the illumination is known, the aerosol number density and size distribution can be obtained. Experiments with alumina particles of given size distributions indicate that the method works accurately. One set of a typical experiment with 3.0-micrometer Al2O3 particles is presented, which shows that the measured size distribution peaks at approximately 3.0 micrometer.

Deepak, A.↗

Retrieval of stratospheric aerosol size distribution from atmospheric extinction of solar radiation at two wavelengths

A parametric study is presented of the effects of the size distribution and composition of stratospheric aerosols on the value R, the ratio of the extinction of solar radiation at wavelength 0.45 micron to the extinction at wavelength 1.0 micron. The aerosol size distributions under study comprise nine analytical expressions, including most of the stratospheric aerosol models used by investigators. The aerosol compositions considered are the supercooled sulfuric-acid droplets, with different weight percentages of H2SO4 in the aerosol. It is found that whereas R is not very sensitive to either the composition or the radii limits of the stratospheric aerosols under consideration, it is quite sensitive to the value of the variable parameter governing the mode radius of the size distribution of aerosol particles. The results of the parametric study underlie the method proposed here of retrieving the size distribution of aerosol particles in the stratosphere from the experimental results of the extinction of solar radiation at two wavelengths.

Yue, G. K.↗

Size distribution and scattering phase function of aerosol particles retrieved from sky brightness measurements

Ground-based measurements of the solar transmission and sky radiance in a horizontal plane through the Sun are taken in several geographical regions and aerosol types: dust in a desert transition zone in Israel, sulfate particles in Eastern and Western Europe, tropical aerosol in Brazil, and mixed continental/maritime aerosol in California. Stratospheric aerosol was introduced after the eruption of Mount Pinatubo in June 1991. Therefore measurements taken before the eruption are used to analyze the properties of tropospheric aerosol; measurements from 1992 are also used to detect the particle size and concentration of stratospheric aerosol. The measurements are used to retrieve the size distribution and the scattering phase function at large scattering angles of the undisturbed aerosol particles. The retrieved properties represent an average on the entire atmospheric column. A comparison between the retrieved phase function for a scattering angle of 120 deg, with phase function predicted from the retrieved size distribution, is used to test the assumption of particle homogeneity and sphericity in radiative transfer models (Mie theory). The effect was found to be small (20% +/- 15%). For the stratospheric aerosol (sulfates), as expected, the phase function was very well predicted using the Mie theory. A model with a power law distribution, based on the spectral dependence of the optical thickness, alpha, cannot estimate accurately the phase function (up to 50% error for lambda = 0.87 microns). Before the Pinatubo eruption the ratio between the volumes of sulfate and coarse particles was very well correlated with alpha. The Pinatubo stratospheric aerosol destroyed this correlation. The aerosol optical properties are compared with analysis of the size, shape, and composition of the individual particles by electron microscopy of in situ samples. The measured volume size distribution before the injection of stratospheric aerosol consistently show two modes, sulfate particles with r(sub m) less than 0.2 microns and coarse paritcles with r(sub m) greater than 0.7 microns. The 'window' in the tropospheric aerosol in this radius range was used to observe a stable stratospheric aerosol in 1992, with r(sub m) approximately 0.5 microns. A combination of such optical thickness and sky measurements can be used to assess the direct forcing and the climatic impact of aerosol. Systematic inversion for the key aerosol types (sulfates, smoke, dust, and maritime aerosol) of the size distribution and phase function can give the relationship between the aerosol physical and optical properties that can be used to compute the radiative forcing. This forcing can be validated in dedicated field experiments.

Kaufman, Y. J.↗

Rapid Measurements of Aerosol Ionic Composition and 3-10 nm Particle Size Distributions On The NASA P3 To Better Quantify Processes Affecting Aerosols Advected From East Asia

The Particle Into Liquid Sample (PILS) was deployed on the NASA P3 for airborne measurements of fine particle ionic chemical composition. The data have been quality assured and reside in the NASA data archive. We have analyzed our data to characterize the sources and atmospheric processing of fine aerosol particles advected from the region during the experiments. Fine particle water-soluble potassium was found to serve as a useful aerosol tracer for biomass smoke. Ratios of PILS potassium to sulfate are used as a means of estimating the percent contribution of biomass burning to fine particle mass in mixed plumes advecting from Asia. The high correlations between K+ and NO3(sup -) and NH4(sup +)' indicated that biomass burning was a significant source of these aerosol compounds in the region. It is noteworthy that the air mass containing the highest concentrations of fine particles recorded in all of ACE-Asia and TRACE-P appeared to be advecting from the Bejing/Tientsin urban region and also had the highest K(+), NO3(sup -) and NH4(sup +) concentrations of both studies. Based on K+/SO4(sup 2-) ratio's, we estimated that the plume was composed of approx. 60% biomass burning emissions, possibly from the use of bio-fuels in the urban regions.

Weber, Rodney J.↗

Individual Aerosol Particles from Biomass Burning in Southern Africa: Compositions and Size Distributions of Carbonaceous Particles - 1

Individual aerosol particles in smoke plumes from biomass fires and in regional hazes in southern Africa were studied using analytical transmission electron microscopy (TEM), which allowed detailed characterization of carbonaceous particle types in smoke and determination of changes in particle properties and concentrations during smoke aging. Based on composition, morphology, and microstructure, three distinct types of carbonaceous particles were present in the smoke: organic particles with inorganic (K-salt) inclusions, tar ball particles, and soot. The relative number concentrations of organic particles were largest in young smoke, whereas tar balls were dominant in a slightly aged (1 hour) smoke from a smoldering fire. Flaming fires emitted relatively more soot particles than smoldering fires, but soot was a minor constituent of all studied plumes. Further aging caused the accumulation of sulfate on organic and soot particles, as indicated by the large number of internally mixed organic/sulfate and soot/sulfate particles in the regional haze. Externally mixed ammonium sulfate particles dominated in the boundary layer hazes, whereas organic/sulfate particles were the most abundant type in the upper hazes. Apparently, elevated haze layers were more strongly affected by biomass smoke than those within the boundary layer. Based on size distributions and the observed patterns of internal mixing, we hypothesize that organic and soot particles are the cloud-nucleating constituents of biomass smoke aerosols. Sea-salt particles dominated in the samples taken in stratus clouds over the Atlantic Ocean, off the coast of Namibia, whereas a distinct haze layer above the clouds consisted of aged biomass smoke particles.

Posfai, Mihaly↗

A numerical determination of the evolution of cloud drop spectra due to condensation on natural aerosol particles

The time variation in size of aerosol particles growing by condensation is studied numerically by means of an air parcel model which allows entrainment of air and aerosol particles. Particles of four types of aerosols typically occurring in atmospheric air masses were considered. The present model circumvents any assumption about the size distribution and chemical composition of the aerosol particles by basing the aerosol particle growth on actually observed size distributions and on observed amounts of water taken up under equilibrium by a deposit of the aerosol particles. Characteristic differences in the drop size distribution, liquid water content and supersaturation were found for the clouds which evolved from the four aerosol types considered.

Lee, I. Y.↗

Intercomparison and Evaluation of Global Aerosol Microphysical Properties Among Aerocom Models of a Range of Complexity

Many of the next generation of global climate models will include aerosol schemes which explicitly simulate the microphysical processes that determine the particle size distribution. These models enable aerosol optical properties and cloud condensation nuclei (CCN) concentrations to be determined by fundamental aerosol processes, which should lead to a more physically based simulation of aerosol direct and indirect radiative forcings. This study examines the global variation in particle size distribution simulated by 12 global aerosol microphysics models to quantify model diversity and to identify any common biases against observations. Evaluation against size distribution measurements from a new European network of aerosol supersites shows that the mean model agrees quite well with the observations at many sites on the annual mean, but there are some seasonal biases common to many sites. In particular, at many of these European sites, the accumulation mode number concentration is biased low during winter and Aitken mode concentrations tend to be overestimated in winter and underestimated in summer. At high northern latitudes, the models strongly underpredict Aitken and accumulation particle concentrations compared to the measurements, consistent with previous studies that have highlighted the poor performance of global aerosol models in the Arctic. In the marine boundary layer, the models capture the observed meridional variation in the size distribution, which is dominated by the Aitken mode at high latitudes, with an increasing concentration of accumulation particles with decreasing latitude. Considering vertical profiles, the models reproduce the observed peak in total particle concentrations in the upper troposphere due to new particle formation, although modelled peak concentrations tend to be biased high over Europe. Overall, the multimodel- mean data set simulates the global variation of the particle size distribution with a good degree of skill, suggesting that most of the individual global aerosol microphysics models are performing well, although the large model diversity indicates that some models are in poor agreement with the observations. Further work is required to better constrain size-resolved primary and secondary particle number sources, and an improved understanding of nucleation an growth (e.g. the role of nitrate and secondary organics) will improve the fidelity of simulated particle size distributions.

Cloud physics↗

A Study of the Relationship Between Anthropogenic Sulfate and Cloud Drop Nucleation

The characteristics of the cloud drop size distribution near cloud base are initially determined by the aerosol particles that serve as CCN and by the local updraft velocity. Chemical reactions of the emitted gaseous sulfur compounds due to human activities will alter, through gas-to-particle conversion, the aerosol size distribution, total number, and its chemical composition. Recently, Boucher and Rodhe and Jones et.al have each developed parameterizations relating cloud drop concentration to sulfate mass or aerosol number concentration, respectively, and used them to develop estimates of the indirect forcing by anthropogenic sulfate aerosols. THese parameterizations made use of measure relationships in continental and maritime clouds. However, these relationships are inherently noisy, yielding more than a factor of 2 variation in cloud drop concentration for a given aerosol number (or for a given sulfate mass) concentration. The large spatial and temporal variabilities in the concentration, chemical characteristics, and size distribution of aerosols have made it difficult to develop such a parameterization from data. In this paper, our focus is to develop a means for relating the predicted anthropogenic sulfate mass to cloud drop number concentration over the range of expected conditions associated with continental and marine aerosol. We start with an assumed pre-existing particle size distribution and develop an approximation of the altered distribution after addition of anthropogenic sulfate. We thereby develop a conservative estimate of the possible change in cloud drop number concentration due to anthropogenic sulfate.

Chuang, Catherine C.↗

Aerosol-Cloud Interactions during Tropical Deep Convection: Evidence for the Importance of Free Tropospheric Aerosols

NASA's 2002 CRYSTAL-FACE field experiment focused on the formation and evolution of tropical cirrus cloud systems in southern Florida. Multiple aircraft extensively sampled cumulonimbus dynamical and microphysical properties, as well as characterizing ambient aerosol populations both inside and outside the full depth of the convective column. On July 18, unique measurements were taken when a powerful updraft was traversed directly by aircraft, providing a window into the primary source region of cumulonimbus anvil crystals. Observations of the updraft, entered at approximately l0 km altitude and -34 C, indicated more than 200 cloud particles per mL at vertical velocities exceeding 20 m/s and the presence of significant condensation nuclei and liquid water within the core. In this work, aerosol and cloud phase observations are integrated by simulating the updraft conditions using a large-eddy resolving model with 3 explicit multiphase microphysics, including treatment of size-resolved aerosol fields, aerosol activation and freezing, and evaporation of cloud particles back to the aerosol phase. Simulations were initialized with observed thermodynamic and aerosol size distributions profiles and convection was driven by surface fluxes assimilated from the ARPS forecast model. Model results are consistent with the conclusions that most crystals are homogeneously frozen droplets and that entrained free tropospheric aerosols may contribute a significant fraction of the crystals. Thus most anvil crystals appear to be formed aloft in updraft cores, well above cloud base. These conclusions are supported by observations of hydrometeor size distribution made while traversing the dore, as well as aerosol and cloud particle size distributions generally observed by aircraft below 4km and crystal properties generally observed by aircraft above 12km.

Ackerman, A.↗

Simulation of the Aerosol Size Distribution Using a Neural Network Surrogate for the Modal Aerosol Module (MAM7)

One objective of atmospheric simulations is to quantify the distribution of aerosols and their properties. Accurate parameterizations of the processes governing aerosol mass, particle number, and particle size distribution are important for predicting the Earth’s net radiative balance and aerosol-cloud interactions. The Modal Aerosol Module (MAM7) is a two-moment aerosol model that simulates mass, number, and size distribution of seven modes comprised of internally mixed aerosol species. The two-moment scheme adds significant computational expense but allows for the prediction of varying particle size distribution relative to the bulk method which predicts only total mass. In this work, we developed a neural network surrogate model for MAM7 (MAMnet) to predict the aerosol number concentration in NASA’s Global Earth Observing System (GEOS) without adding prohibitive computational expense. MAMnet, can be driven by output from a single moment, mass-based, aerosol scheme (Goddard Chemistry Aerosol and Radiation model (GOCART)) or from reanalysis products (Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2)). MAMnet was trained using number concentrations from a 5-year GEOS/MAM7 simulation at 1-degree horizontal resolution and using the total mass calculated across modes as inputs, as well as temperature and air density. The model architecture for MAMnet was based on AlexNet, the 2012 winner of the ImageNet Large Scale Visual Recognition Challenge. While some modifications were necessary to accommodate our problem, important aspects of the network were preserved. MAMnet was able to reproduce zonal dynamics and spatial distributions of the aerosol number concentration however predictability in the upper troposphere was poor.

Katherine H Breen↗

High-Precision Measurement of Eu/Eu* in Geological Glasses via LA-ICP-MS Analysis

Elemental fractionation during laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) analysis has been historically documented between refractory and volatile elements. In this work, however, we observed fractionation between light rare earth elements (LREEs) and heavy rare earth elements (HREEs) when using ablation strategies involving large spot sizes (greater than 100 millimeters) and line scanning mode. In addition: (1) ion yields decrease when using spot sizes above 100 millimeters; (2) (Eu/Eu*)(sub raw) (i.e. Europium anomaly) positively correlates with carrier gas (He) flow rate, which provides control over the particle size distribution of the aerosol reaching the ICP; (3) (Eu/Eu*)(sub raw) shows a positive correlation with spot size, and (4) the changes in REE signal intensity, induced by the He flow rate change, roughly correlate with REE condensation temperatures. The REE fractionation is likely driven by the slight but significant difference in their condensation temperatures. Large particles may not be completely dissociated in the ICP and result in preferential evaporation of the less refractory LREEs and thus non-stoichiometric particle-ion conversion. This mechanism may also be responsible for Sm-Eu-Gd fractionation as Eu is less refractory than Sm and Gd. The extent of fractionation depends upon the particle size distribution of the aerosol, which in turn is influenced by the laser parameters and matrix. Ablation pits and lines defined by low aspect ratios produce a higher proportion of large particles than high aspect ratio ablation, as confirmed by measurements of particle size distribution in the laser induced aerosol. Therefore, low aspect ratio ablation introduces particles that cannot be decomposed and/or atomized by the ICP and thus results in exacerbated elemental fractionation. Accurate quantification of REE concentrations and Eu/Eu* requires reduction of large particle production during laser ablation. For the reference materials analyzed in this work, the 100 millimeters spot measurements of Eu/Eu* agreed with GeoRem preferred values within 3 percent. Our long-term analyses of Eu/Eu* in MPI-DING glass KL-2G and USGS glass BIR-1G were reproducible at 3 percent (2 RSD).

geological glasses↗

Aerosol Seasonal Variations over Urban-Industrial Regions in Ukraine According to AERONET and POLDER Measurements

The paper presents an investigation of aerosol seasonal variations in several urban-industrial regions in Ukraine. Our analysis of seasonal variations of optical and physical aerosol parameters is based on the sun-photometer 2008-2013 data from two urban ground-based AERONET (AErosol RObotic NETwork) sites in Ukraine (Kyiv, Lugansk) as well as on satellite POLDER instrument data for urban-industrial areas in Ukraine. We also analyzed the data from one AERONET site in Belarus (Minsk) in order to compare with the Ukrainian sites. Aerosol amount and optical depth (AOD) values in the atmosphere columns over the large urbanized areas like Kyiv and Minsk have maximum values in the spring (April-May) and late summer (August), whereas minimum values are observed in late autumn. The results show that fine-mode particles are most frequently detected during the spring and late summer seasons. The analysis of the seasonal AOD variations over the urban-industrial areas in the eastern and central parts of Ukraine according to both ground-based and POLDER data exhibits the similar traits. The seasonal variation similarity in the regions denotes the resemblance in basic aerosol sources that are closely related to properties of aerosol particles. The behavior of basic aerosol parameters in the western part of Ukraine is different from eastern and central regions and shows an earlier appearance of the spring and summer AOD maxima. Spectral single-scattering albedo, complex refractive index and size distribution of aerosol particles in the atmosphere column over Kyiv have different behavior for warm (April-October) and cold seasons. The seasonal features of fine and coarse aerosol particle behavior over the Kyiv site were analyzed. A prevailing influence of the fine-mode particles on the optical properties of the aerosol layer over the region has been established. The back-trajectory and cluster analysis techniques were applied to study the seasonal back trajectories and prevailing directions of the arrived air mass for the Kyiv and Minsk sites.

Ukraine↗

TPSAS-NF1676L-34013-DND

Currently, many experiments pursuing comprehensive characterization of the atmosphere include coordinated observations by both lidar and polarimeters in order to obtain important complimentary information about aerosol properties. The most advanced passive observations by space-based multi-angle polarimeters are sensitive to the properties of aerosol in total atmospheric column, but have very limited sensitivity to vertical structure of the atmosphere. Polarimeter observations can be used not only for retrieval of aerosol optical thickness, but also for deriving microphysical information about aerosol particle shape, size distribution, complex refractive index, and the properties of underlying surface (Dubovik et al., 2019). In a contrast, the lidar observations of atmospheric responses from different altitudes to laser pulses are designed to provide vertical profiles of atmospheric characteristics. Here we present the recent advancement in GRASP algorithm (Generalized Aerosol Retrieval of Atmospheric and Surface Properties) (Dubovik et al., 2011, 2014) that allows simultaneous inversion of co-incident lidar and polarimeter spaceborne observations and derives a united set of vertically resolved aerosol and surface parameters. Such synergetic retrieval is an extension to satellite data of the approach for synergetic processing of active and passive measurements developed earlier by (Lopatin et al., 2013) for ground-based observations. Another addition to these developments is the inclusion of Raman-shifted and volume depolarization backscattering observations that improve sensitivity to the vertical properties of aerosol, while polarimetric observations provide sufficient constraints on aerosol type and loading that generally are missing in lidar signals. The potential and limitations of such synergetic processing is illustrated by application to co-incident PARASOL and CALIPSO data.

Anton Lopatin↗

Inverse atmospheric radiative transfer problems - A nonlinear minimization search method of solution

The paper studies the inversion of the radiative transfer equation describing the interaction of electromagnetic radiation with atmospheric aerosols. The interaction can be considered as the propagation in the aerosol medium of two light beams: the direct beam in the line-of-sight attenuated by absorption and scattering, and the diffuse beam arising from scattering into the viewing direction, which propagates more or less in random fashion. The latter beam has single scattering and multiple scattering contributions. In the former case and for single scattering, the problem is reducible to first-kind Fredholm equations, while for multiple scattering it is necessary to invert partial integrodifferential equations. A nonlinear minimization search method, applicable to the solution of both types of problems has been developed, and is applied here to the problem of monitoring aerosol pollution, namely the complex refractive index and size distribution of aerosol particles.

Fymat, A. L.↗

The NASA-AMES Research Center Stratospheric Aerosol Model. 1. Physical Processes and Computational Analogs

A time-dependent one-dimensional model of the stratospheric sulfate aerosol layer is presented. In constructing the model, a wide range of basic physical and chemical processes are incorporated in order to avoid predetermining or biasing the model predictions. The simulation, which extends from the surface to an altitude of 58 km, includes the troposphere as a source of gases and condensation nuclei and as a sink for aerosol droplets. The size distribution of aerosol particles is resolved into 25 categories with particle radii increasing geometrically from 0.01 to 2.56 microns such that particle volume doubles between categories.

Turco, R. P.↗