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At least 235 records · Page 13

How We Can Constrain Aerosol Type Globally

In addition to aerosol number concentration, aerosol size and composition are essential attributes needed to adequately represent aerosol-cloud interactions (ACI) in models. As the nature of ACI varies enormously with environmental conditions, global-scale constraints on particle properties are indicated. And although advanced satellite remote-sensing instruments can provide categorical aerosol-type classification globally, detailed particle microphysical properties are unobtainable from space with currently available or planned technologies. For the foreseeable future, only in situ measurements can constrain particle properties at the level-of-detail required for ACI, as well as to reduce uncertainties in regional-to-global-scale direct aerosol radiative forcing (DARF). The limitation of in situ measurements for this application is sampling. However, there is a simplifying factor: for a given aerosol source, in a given season, particle microphysical properties tend to be repeatable, even if the amount varies from day-to-day and year-to-year, because the physical nature of the particles is determined primarily by the regional environment. So, if the PDFs of particle properties from major aerosol sources can be adequately characterized, they can be used to add the missing microphysical detail the better sampled satellite aerosol-type maps. This calls for Systematic Aircraft Measurements to Characterize Aerosol Air Masses (SAM-CAAM). We are defining a relatively modest and readily deployable, operational aircraft payload capable of measuring key aerosol absorption, scattering, and chemical properties in situ, and a program for characterizing statistically these properties for the major aerosol air mass types, at a level-of-detail unobtainable from space. It is aimed at: (1) enhancing satellite aerosol-type retrieval products with better aerosol climatology assumptions, and (2) improving the translation between satellite-retrieved aerosol optical properties and species-specific aerosol mass and size that are tracked in aerosol transport and climate models used to assess aerosol forcing and its anthropogenic components. This presentation will summarize where we stand on the development of the SAM-CAAM concept.

DARF↗

Evaluation of Observed and Modelled Aerosol Lifetimes Using Radioactive Tracers of Opportunity and an Ensemble of 19 Global Models

Aerosols have important impacts on air quality and climate, but the processes affecting their removal from the atmosphere are not fully understood and are poorly constrained by observations. This makes modelled aerosol lifetimes uncertain. In this study, we make use of an observational constraint on aerosol lifetimes provided by radionuclide measurements and investigate the causes of differences within a set of global models. During the Fukushima Dai-Ichi nuclear power plant accident of March 2011, the radioactive isotopes cesium-137 (Cs-137) and xenon-133 (Xe-133) were released in large quantities. Cesium attached to particles in the ambient air, approximately according to their available aerosol surface area. Cs-137 size distribution measurements taken close to the power plant suggested that accumulation mode (AM) sulfate aerosols were the main carriers of cesium. Hence, Cs-137 can be used as a proxy tracer for the AM sulfate aerosol's fate in the atmosphere. In contrast, the noble gas Xe-133 behaves almost like a passive transport tracer. Global surface measurements of the two radioactive isotopes taken over several months after the release allow the derivation of a lifetime of the carrier aerosol. We compare this to the lifetimes simulated by 19 different atmospheric transport models initialized with identical emissions of Cs-137that were assigned to an aerosol tracer with each model's default properties of AM sulfate, and Xe-133 emissions that were assigned to a passive tracer. We investigate to what extent the modelled sulfate tracer can reproduce the measurements, especially with respect to the observed loss of aerosol mass with time. Modelled Cs-137and Xe-133 concentrations sampled at the same location and times as station measurements allow a direct comparison between measured and modelled aerosol lifetime. The e-folding lifetime e, calculated from station measurement data taken between 2 and 9 weeks after the start of the emissions, is 14.3 days (95% confidence interval 13.1-15.7 days). The equivalent modelled e lifetimes have a large spread, varying between 4.8 and 26.7 days with a model median of 9.42.3 days, indicating too fast a removal in most models. Because sufficient measurement data were only available from about 2 weeks after the release, the estimated lifetimes apply to aerosols that have undergone long-range transport, i.e. not for freshly emitted aerosol. However, modelled instantaneous lifetimes show that the initial removal in the first 2 weeks was quicker (lifetimes between 1 and 5 days) due to the emissions occurring at low altitudes and co-location of the fresh plume with strong precipitation. Deviations between measured and modelled aerosol lifetimes are largest for the northernmost stations and at later time periods, suggesting that models do not transport enough of the aerosol towards the Arctic. The models underestimate passive tracer (Xe-133) concentrations in the Arctic as well but to a smaller extent than for the aerosol (Cs-137) tracer. This indicates that in addition to too fast an aerosol removal in the models, errors in simulated atmospheric transport towards the Arctic in most models also contribute to the underestimation of the Arctic aerosol concentrations.

Radioactive isotopes↗

Synergistic Use of Hyperspectral UV-Visible OMI and Broadband Meteorological Imager MODIS Data for a Merged Aerosol Product

The retrieval of optimal aerosol datasets by the synergistic use of hyperspectral ultraviolet(UV)–visible and broadband meteorological imager (MI) techniques was investigated. The Aura Ozone Monitoring Instrument (OMI) Level 1B (L1B) was used as a proxy for hyperspectral UV–visible instrument data to which the Geostationary Environment Monitoring Spectrometer (GEMS) aerosol algorithm was applied. Moderate-Resolution Imaging Spectroradiometer (MODIS) L1B and dark target aerosol Level 2 (L2) data were used with a broadband MI to take advantage of the consistent time gap between the MODIS and the OMI. First, the use of cloud mask information from the MI infrared (IR) channel was tested for synergy. High-spatial-resolution and IR channels of the MI helped mask cirrus and sub-pixel cloud contamination of GEMS aerosol, as clearly seen in aerosol optical depth (AOD) validation with Aerosol Robotic Network (AERONET) data. Second, dust aerosols were distinguished in the GEMS aerosol-type classification algorithm by calculating the total dust confidence index (TDCI) from MODIS L1B IR channels. Statistical analysis indicates that the Probability of Correct Detection (POCD) between the forward and inversion aerosol dust models (DS) was increased from 72% to 94% by use of the TDCI for GEMS aerosol-type classification, and updated aerosol types were then applied to the GEMS algorithm. Use of the TDCI for DS type classification in the GEMS retrieval procedure gave improved single-scattering albedo (SSA) values for absorbing fine pollution particles (BC) and DS aerosols. Aerosol layer height (ALH) retrieved from GEMS was compared with Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) data, which provides high-resolution vertical aerosol profile information. The CALIOP ALH was calculated from total attenuated backscatter data at 1064 nm, which is identical to the definition of GEMS ALH. Application of the TDCI value reduced the median bias of GEMS ALH data slightly. The GEMS ALH bias approximates zero, especially for GEMS AOD values of>~0.4 and GEMS SSA values of<~0.95.Finally, the AOD products from the GEMS algorithm and MI were used in aerosol merging with the maximum-likelihood estimation method, based on a weighting factor derived from the standard deviation of the original AOD products. With the advantage of the UV–visible channel in retrieving aerosol properties over bright surfaces, the combined AOD products demonstrated better spatial data availability than the original AOD products, with comparable accuracy. Furthermore, pixel-level error analysis of GEMS AOD data indicates improvement through MI synergy.

aerosol↗

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.↗

Measurements and Modeling of Aerosol Absorption and Single Scattering Albedo at Ambient Relative Hum

Uncertainties in the aerosol single scattering albedo have been identified to be an important source of errors in current large-scale model estimates of the direct aerosol radiative forcing of climate. A number of investigators have obtained estimates of the single scattering albedo from a variety of remote sensing and in situ measurements during aerosol field experiments. During the Tropospheric Aerosol Radiative Forcing Observational Experiment (TARFOX, 1996) for example, estimates of the aerosol single scattering albedo were obtained (1) as a best-fit parameter in comparing radiative flux changes measured by airborne pyranometer to those computed from independently measured aerosol properties; (2) from estimates of the aerosol complex index of refraction derived using a combination of airborne sunphotometer, lidar backscatter and in situ size distribution measurements; and (3) from airborne measurements of aerosol scattering and absorption using nephelometers and absorption photometers. In this paper, we briefly compare the results of the latter two methods for two TARFOX case studies, since those techniques provide height-resolved information about the aerosol single scattering albedo. Estimates of the aerosol single scattering albedo from nephelometer and absorption photometer measurements require knowledge of the scattering and absorption humidification (i.e., the increase in these properties in response to an increase in ambient relative humidity), since both measurements are usually carried out at a relative humidity different from the ambient atmosphere. In principle, the scattering humidification factor can be measured, but there is currently no technique widely available to measure the absorption of an aerosol sample as a function of relative humidity. Frequently, for lack of better knowledge, the absorption humidification is assumed to be unity (meaning that there is no change in aerosol absorption due to an increase in ambient relative humidity). This assumption then enters the estimate of the single scattering albedo at ambient relative humidity. To investigate the validity of this assumption we have carried out modeling studies of the absorption humidification factor, assuming that the aerosols contain an insoluble soot core and a coating which determines its hygroscopic growth behavior. The aerosol optical properties are then computed on the basis of the shell/core particle morphology using a Mie-code for concentric shells. From basic physical principles, it is conceivable that aerosol absorption increases when an atmospheric aerosol particle collects a non-absorbing shell, since the soot core is then exposed to an increased (focused) electric field strength. Indeed, our preliminary modeling studies show that the absorption of an atmospheric aerosol particle composed of a soot core and an aqueous sulfuric acid shell may increase by a factor of 50% due to a change in ambient relative humidity from 30 to 95%. We will show how this increased absorption is a function of the initial particle size and soot mass fraction.

Redemann, J.↗

The Use of Satellite-Measured Aerosol Optical Depth to Constrain Biomass Burning Emissions Source Strength in a Global Model GOCART

Small particles in the atmosphere, called "atmospheric aerosol" have a direct effect on Earth climate through scattering and absorbing sunlight, and also an indirect effect by changing the properties of clouds, as they interact with solar radiation as well. Aerosol typically stays in the atmosphere for several days, and can be transported long distances, affecting air quality, visibility, and human health not only near the source, but also far downwind. Smoke from vegetation fires is one of the main sources of atmospheric aerosol; other sources include anthropogenic pollution, dust, and sea salt. Chemistry transport models (CTMs) are among the major tools for studying the atmospheric and climate effects of aerosol. Due to the considerable variation of aerosol concentrations and properties on many temporal and spatial scales, and the complexity of the processes involved, the uncertainties in aerosol effects on climate are large, as is featured in the latest report of Intergovernmental Panel on Climate Change (IPCC) in 2007. Reducing this uncertainty in the models is very important both for predicting future climate scenarios and for regional air quality forecasting and mitigation. During vegetation fires, also called biomass burning (BB) events, complex mixture of gases and particles is emitted. The amount of BB emissions is usually estimated taking into account the intensity and size of the fire and the properties of burning vegetation. These estimates are input into CTMs to simulate BB aerosol. Unfortunately, due to large variability of fire and vegetation properties, the quantity of BB emissions is very difficult to estimate and BB emission inventories provide numbers that can differ by up to the order of magnitude in some regions. Larger uncertainties in data input make uncertainties in model output larger as well. A powerful way to narrow the range of possible model estimates is to compare model output to observations. We use satellite observations of aerosol properties, specifically aerosol optical depth, which is directly proportional to the amount of aerosol in the atmosphere, and compare it to the model output. Assuming the model represents aerosol transport and particle properties correctly, the amount of BB emissions determines the simulated aerosol optical depth. In this study, we explore the regional performance of 13 commonly used emission estimates. These are each input to global Goddard Chemistry Aerosol Radiation and Transport (GOCART) model. We then evaluate how well each emission estimate reproduces the smoke aerosol optical depth measured by the MODIS instrument. We compared GOCART-simulate aerosol optical depth with that measured from the satellite for 124 fire cases around the world during 2006 and 2007. We summarize the regional performance of each emission inventory and discuss reasons for their differences by considering the assumptions made during their development. We also show that because stronger wind disperses smoke plumes more readily, in cases with stronger wind, a larger increase in emission amount is needed to increase aerosol optical depth. In quiet, low-wind-speed environments, BB emissions produce a more significant increase in aerosol optical depth, other things being equal. Using the region-specific, quantitative relationships derived in our paper, together with the wind speed obtained from another source for a given fire case, we can constrain the amount of emission required in the model to reproduce the observations. The results of this paper are useful to the developers of BB emission inventories, as they show the strengths and weaknesses of individual emission inventories in different regions of the globe, and also for modelers who use these inventories and wish to improve their model results.

Petrenko, Mariya↗

Evaluation of GEOS Aerosols Using CAMP2Ex Observations

Biomass burning aerosol impacts aspects of the atmosphere and Earth system through direct and semi-direct effects, as well as influencing air quality. Despite its importance, the representation of biomass burning aerosol is not always accurate in numerical weather prediction and climate models or reanalysis products. Using observations collected as part of the Cloud, Aerosol and Monsoon Processes Philippines Experiment (CAMP2Ex) in August through October of 2019, aerosol concentration and optical properties are evaluated within the Goddard Earth Observing System (GEOS) and its underlying aerosol module, GOCART. In the operational configuration, GEOS assimilates aerosol optical depth observations at 550 nm from AERONET and MODIS to constrain aerosol fields. Particularly for biomass burning aerosol, without the assimilation of aerosol optical depth, aerosol extinction is underestimated compared to observations collected in the Philippines region during the CAMP2Ex campaign. The assimilation process adds excessive amounts of carbon to account for the underestimated extinction, resulting in positive biases in the mass of black and organic carbon, especially within the boundary layer, relative to in situ observations from the Langley Aerosol Research Group Experiment. Counteracting this, GEOS is deficient in sulfate and nitrate aerosol just above the boundary layer. Aerosol extinction within GEOS is a function of the mass of different aerosol species, the ambient relative humidity, the assumed spectral optical properties, and particle size distribution per species. The relationship between dry and ambient extinction in GEOS reveals that hygroscopic growth is too high within the model for biomass burning aerosol. An additional concern lies in the assumed particle size distribution for GEOS, which has a single mode radius that is too small for organic carbon. Variability in the observed particle size distribution for biomass burning aerosol within a single flight also illuminates the fact that a single assumed particle size distribution is not sufficient and that for a proper representation, a more advanced aerosol module within GEOS may be necessary.

Allison Collow↗

Application of Satellite and Ground-based Data to Investigate the UV Radiative Effects of Australian Aerosols

An understanding of the effect of aerosols on biologically- and photochemically-active UV radiation reaching the Earth's surface is important for many ongoing climate, biophysical, and air pollution studies. In particular, estimates of the UV characteristics of the most common Australian aerosols will be valuable inputs to UV Index forecasts, air quality studies, and assessments of the impact of regional environmental changes. By analyzing climatological distributions of Australian aerosols we have identified sites where co-located ground-based UV-B and ozone measurements were available during episodes of relatively high aerosol activity. Since at least June 2003, surface UV global irradiance spectra (285-450 nm) have been measured routinely at Darwin and Alice Springs in Australia by the Australian Bureau of Meteorology (BoM). Using colocated sunphotometer measurements at Darwin and Alice Springs, we identified several episodes of relatively high aerosol activity. Aerosol air mass types were analyzed from sunphotometer-derived angstrom parameter, MODIS fire maps and MISR aerosol property retrievals. To assess aerosol effects we compared the measured UV irradiances for aerosol-loaded and clear-sky conditions with each other and with irradiances simulated using the libRadtran radiative transfer model for aerosol-free conditions. We found that for otherwise similar atmospheric conditions, smoke aerosols over Darwin reduced the surface UV irradiance by as much as 40-50% at 290-300 nm and 20-25% at 320-400 nm near active fires (aerosol optical depth, AOD, at 500 nm approximately equal to 0.6). Downwind of fires, the smoke aerosols over Darwin reduced the surface irradiance by 15-25% at 290-300 nm and approximately 10% at 320-350 nm (AOD at 500 nm approximately equal to 0.2). The effect of smoke increased with decrease of wavel strongest in the UV-B. The aerosol attenuation factors calculated for the selected cases suggest smoke over Darwin has an effect on surface 340-380 nm irradiances that is comparable to that produced by smoke over Sub-Saharan Africa. Dust activity was very low at Alice Springs during 2004, therefore we were not able to identify strong dust events to fully assess the UVeffect of dust. For the cases studied, smoke aerosols seem to produce a stronger reduction in surface UV irradiances than dust aerosols.

UV surface irradiances↗

An Evaluation of Biomass Burning Aerosol Mass, Extinction, and Size Distribution in Geos Using Observations From Camp2EX

Biomass burning aerosol impacts aspects of the atmosphere and Earth system through radiative forcing, serving as cloud condensation nuclei, and air quality. Despite its importance, the representation of biomass burning aerosol is not always accurate in numerical weather prediction and climate models or reanalysis products. Using observations collected as part of the Cloud, Aerosol and Monsoon Processes Philippines Experiment (CAMP2Ex) in August through October of 2019, aerosol concentration and optical properties are evaluated within the Goddard Earth Observing System (GEOS) and its underlying aerosol module, GOCART. In the operational configuration, GEOS assimilates aerosol optical depth observations at 550 nm to constrain aerosol fields. Particularly for biomass burning aerosol, without the assimilation of aerosol optical depth, aerosol extinction is underestimated compared to observations collected in the Philippines region during the CAMP2Ex campaign. The assimilation process adds excessive amounts of carbon to account for the underestimated extinction, resulting in positive biases in the mass of black and organic carbon, especially within the boundary layer, relative to in situ observations from the Langley Aerosol Research Group Experiment. Counteracting this, GEOS is deficient in sulphate and nitrate aerosol just above the boundary layer. Aside from aerosol mass, extinction within GEOS is a function of ambient relative humidity and an assumed particle size distribution. The relationship between dry and ambient extinction in GEOS reveals that hygroscopic growth is too aggressive within the model for biomass burning aerosol. An additional concern lies in the assumed particle size distribution for GEOS, which has a mode radius that is too small for organic carbon. Variability in the observed particle size distribution for biomass burning aerosol within a single flight also illuminates the fact that a single assumed particle size distribution is not sufficient and that for a proper representation, a more advanced aerosol module with GEOS may be necessary.

Aerosol Mass↗

Preliminary Results from an Assimilation of TOMS Aerosol Observations Into the GOCART Model

At NASA Goddard we are developing a global aerosol data assimilation system that combines advances in remote sensing and modeling of atmospheric aerosols. The goal is to provide high resolution, 3-D aerosol distributions to the research community. Our first step is to develop a simple assimilation system for Saharan mineral aerosol. The Goddard Chemistry and Aerosol Radiation model (GOCART) provides accurate 3-D mineral aerosol size distributions that compare well with TOMS satellite observations. Surface, mobilization, wet and dry deposition, convective and long-range transport are all driven by assimilated fields from the Goddard Earth Observing System Data Assimilation System, GEOS-DAS. Our version of GOCART transports sizes from.08-10 microns and only simulates Saharan dust. TOMS radiance observations in the ultra violet provide information on the mineral and carbonaceous aerosol fields. We use two main observables in this study: the TOMS aerosol index (AI) which is directly related to the ratio of the 340 and 380 radiances and the 380 radiance. These are sensitive to the aerosol optical thickness, the single scattering albedo and the height of the aerosol layer. The Goddard Aerosol Assimilation System (GAAS) uses the Data Assimilation Office's Physical-space Statistical Analysis System (PSAS) to combine TOMS observations and GOCART model first guess fields. At this initial phase we only assimilate observations into the the GOCART model over regions of Africa and the Atlantic where mineral aerosols dominant and carbonaceous aerosols are minimal, Our preliminary results during summer show that the assimilation with TOMS data modifies both the aerosol mass loading and the single scattering albedo. Assimilated aerosol fields will be compared with assimilated aerosol fields from GOCART and AERONET observations over Cape Verde.

daSilva, Arlindo↗

Evaluation of Daytime Measurements of Aerosols and Water Vapor made by an Operational Raman Lidar over the Southern Great Plains

Raman lidar water vapor and aerosol extinction profiles acquired during the daytime over the Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) site in northern Oklahoma (36.606 N, 97.50 W, 315 m) are evaluated using profiles measured by in situ and remote sensing instruments deployed during the May 2003 Aerosol Intensive Operations Period (IOP). The automated algorithms used to derive these profiles from the Raman lidar data were first modified to reduce the adverse effects associated with a general loss of sensitivity of the Raman lidar since early 2002. The Raman lidar water vapor measurements, which are calibrated to match precipitable water vapor (PWV) derived from coincident microwave radiometer (MWR) measurements were, on average, 5-10% (0.3-0.6 g/m(exp 3) higher than the other measurements. Some of this difference is due to out-of-date line parameters that were subsequently updated in the MWR PWV retrievals. The Raman lidar aerosol extinction measurements were, on average, about 0.03 km(exp -1) higher than aerosol measurements derived from airborne Sun photometer measurements of aerosol optical thickness and in situ measurements of aerosol scattering and absorption. This bias, which was about 50% of the mean aerosol extinction measured during this IOP, decreased to about 10% when aerosol extinction comparisons were restricted to aerosol extinction values larger than 0.15 km(exp -1). The lidar measurements of the aerosol extinction/backscatter ratio and airborne Sun photometer measurements of the aerosol optical thickness were used along with in situ measurements of the aerosol size distribution to retrieve estimates of the aerosol single scattering albedo (omega(sub o)) and the effective complex refractive index. Retrieved values of omega(sub o) ranged from (0.91-0.98) and were in generally good agreement with omega(sub o) derived from airborne in situ measurements of scattering and absorption. Elevated aerosol layers located between about 2.6 and 3.6 km were observed by the Raman lidar on May 25 and May 27. The airborne measurements and lidar retrievals indicated that these layers, which were likely smoke produced by Siberian forest fires, were primarily composed of relatively large particles (r(sub eff) approximately 0.23 micrometers), and that the layers were relatively nonabsorbing (omega(sub o) approximately 0.96-0.98). Preliminary results show that major modifications that were made to the Raman lidar system during 2004 have dramatically improved the sensitivity in the aerosol and water vapor channels and reduced random errors in the aerosol scattering ratio and water vapor retrievals by an order of magnitude.

Ferrare, Richard↗

Assessment of Aerosol Distributions from GEOS-5 Using the CALIPSO Feature Mask

A-train sensors such as MODIS, MISR, and CALIPSO are used to determine aerosol properties, and in the process a means of estimating aerosol type (e.g. smoke vs. dust). Correct classification of aerosol type is important for climate assessment, air quality applications, and for comparisons and analysis with aerosol transport models. The Aerosols-Clouds-Ecosystems (ACE) satellite mission proposed in the NRC Decadal Survey describes a next generation aerosol and cloud suite similar to the current A-train, including a lidar. The future ACE lidar must be able to determine aerosol type effectively in conjunction with modeling activities to achieve ACE objectives. Here we examine the current capabilities of CALIPSO and the NASA Goddard Earth Observing System general circulation model and data assimilation system (GEOS-5), to place future ACE needs in context. The CALIPSO level 2 feature mask includes vertical profiles of aerosol layers classified by type. GEOS-5 provides global 3D aerosol mass for sulfate, sea salt, dust, and black and organic carbon. A GEOS aerosol scene classification algorithm has been developed to provide estimates of aerosol mixtures and extinction profiles along the CALIPSO orbit track. In previous work, initial comparisons between GEOS-5 derived aerosol mixtures and CALIPSO derived aerosol types were presented for July 2007. In general, the results showed that model and lidar derived aerosol types did not agree well in the boundary layer. Agreement was poor over Europe, where CALIPSO indicated the presence of dust and pollution mixtures yet GEOS-5 was dominated by pollution with little dust. Over the ocean in the tropics, the model appeared to contain less sea salt than detected by CALIPSO, yet at high latitudes the situation was reserved. Agreement between CALIPSO and GEOS-5, aerosol types improved above the boundary layer, primarily in dust and smoke dominated regions. At higher altitudes (> 5 km), the model contained aerosol layers not detected by CALIPSO. Here we present new results for a full year study using the new Version 3 CALIPSO data and most recent GEOS-5 model results.

Welton, Ellsworth↗

Explicit Aerosol Correction of OMI Formaldehyde Retrievals

Atmospheric aerosols are significant sources of uncertainty in air mass factor (AMF) calculations for trace gas retrievals using ultraviolet measurements from space. Current trace gas retrievals typically do not consider aerosols explicitly as cloud products partially account for aerosol effects. Here, we propose a new measurement-based approach to correct for aerosols explicitly in the AMF calculation, apply it to Ozone Monitoring Instrument (OMI) formaldehyde (HCHO) retrievals and quantify the aerosol-induced HCHO vertical column density difference for three aerosol types (smoke, dust, and sulfate) during 2006–2007. We use OMI aerosol retrievals for aerosol optical properties and vertical profiles to construct lookup tables of scattering weights as functions of geometry, surface pressure, surface albedo, and aerosol information. The average difference between the National Aeronautics and Space Administration operational OMI HCHO product (not considering aerosols) and the results obtained in this study on a global scale are 27%, 6%, and −0.3% for smoke, dust, and sulfate aerosols, respectively. The region with the largest aerosol effects is East China, where the explicit smoke aerosol correction enhances mean HCHO vertical column densities by 35%, with corrections to individual observations sometimes larger than 100%. The quantified aerosol effects are applicable under clear-sky conditions. This study highlights the need to implement aerosol corrections in the AMF calculation for HCHO retrievals. This is particularly relevant in regions with high levels of pollution where aerosols interfere the most with formaldehyde satellite observations.

Ozone Monitoring Instrument (OMI) formaldehyde (HC↗

Columnar Aerosol Types and Compositions Over Peninsular Southeast Asia Based on Long-Term AERONET Data

Aerosol chemical components such as black carbon (BC) and brown carbon (BrC) regulate aerosol optical properties, which in turn drive the atmospheric radiative forcing estimations due to aerosols. In this study, we used the long-term measurements from AERONET (Aerosol Robotic Network) to better understand the aerosol types and composition with respect to their seasonal and spatial variabilities in peninsular Southeast Asia (PSEA, here defined as Vietnam, Cambodia, Thailand, Laos, and Myanmar). Two methods (i.e., aerosol type cluster and aerosol component retrieval) were applied to determine the aerosol type and chemical composition during the biomass-burning (BB) season. AERONET sites in northern PSEA showed a higher AOD (aerosol optical depth) compared to that of southern PSEA. Differences in land use pattern, geographic location, and weather regime caused much of the aerosol variability over PSEA. Lower single-scattering albedo (SSA) and higher fine-mode fraction (FMF) values were observed in February and March, suggesting the predominance of BB type aerosols with finer and stronger absorbing particles during the dry season. However, we also found that the peak BB month (i.e., March) in northern PSEA may not coincide with the lowest SSA once dust particles have mixed with the other aerosols. Furthermore, we investigated two severe BB events in March of 2014 and 2015, revealing a significant BrC fraction during BB event days. On high AOD days, although the BC fraction was high, the BrC fraction remained low due to lack of aerosol aging. This study highlights the dominance of carbonaceous aerosols in the PSEA atmosphere during the BB season, while also revealing that transported dust particles and BrC aerosol aging may introduce uncertainties into the aerosol radiative forcing calculation.

Sheng-Hsiang Wang↗

AeroCom Phase III Multi-Model Evaluation of the Aerosol Life Cycle and Optical Properties Using Ground and Space-Based Remote Sensing as Well as Surface In Situ Observations

Within the framework of the AeroCom (Aerosol Comparisons between Observations and Models) initiative, the state-of-the-art modelling of aerosol optical properties is assessed from 14 global models participating in the phase III control experiment (AP3). The models are similar to CMIP6/AerChemMIP Earth System Models (ESMs) and provide a robust multi-model ensemble. Inter-model spread of aerosol species lifetimes and emissions appears to be similar to that of mass extinction coefficients (MECs), suggesting that aerosol optical depth (AOD) uncertainties are associated with a broad spectrum of parameterised aerosol processes. Total AOD is approximately the same as in AeroCom phase I (AP1) simulations. However, we find a 50 % decrease in the optical depth (OD) of black carbon (BC), attributable to a combination of decreased emissions and lifetimes. Relative contributions from sea salt (SS) and dust (DU) have shifted from being approximately equal in AP1 to SS contributing about 2∕3 of the natural AOD in AP3. This shift is linked with a decrease in DU mass burden, a lower DU MEC, and a slight decrease in DU lifetime, suggesting coarser DU particle sizes in AP3 compared to AP1. Relative to observations, the AP3 ensemble median and most of the participating models underestimate all aerosol optical properties investigated, that is, total AOD as well as fine and coarse AOD (AODf, AODc), Ångström exponent (AE), dry surface scattering (SCdry), and absorption (ACdry) coefficients. Compared to AERONET, the models underestimate total AOD by ca. 21 % ± 20 % (as inferred from the ensemble median and interquartile range). Against satellite data, the ensemble AOD biases range from −37 % (MODIS-Terra) to −16 % (MERGED-FMI, a multi-satellite AOD product), which we explain by differences between individual satellites and AERONET measurements themselves. Correlation coefficients (R) between model and observation AOD records are generally high (R>0.75), suggesting that the models are capable of capturing spatio-temporal variations in AOD. We find a much larger underestimate in coarse AODc (∼ −45 % ± 25 %) than in fine AODf (∼ −15 % ± 25 %) with slightly increased inter-model spread compared to total AOD. These results indicate problems in the modelling of DU and SS. The AODc bias is likely due to missing DU over continental land masses (particularly over the United States, SE Asia, and S. America), while marine AERONET sites and the AATSR SU satellite data suggest more moderate oceanic biases in AODc. Column AEs are underestimated by about 10 % ± 16 %. For situations in which measurements show AE > 2, models underestimate AERONET AE by ca. 35 %. In contrast, all models (but one) exhibit large overestimates in AE when coarse aerosol dominates (bias ca. +140 % if observed AE < 0.5). Simulated AE does not span the observed AE variability. These results indicate that models overestimate particle size (or underestimate the fine-mode fraction) for fine-dominated aerosol and underestimate size (or overestimate the fine-mode fraction) for coarse-dominated aerosol. This must have implications for lifetime, water uptake, scattering enhancement, and the aerosol radiative effect, which we can not quantify at this moment. Comparison against Global Atmosphere Watch (GAW) in situ data results in mean bias and inter-model variations of −35 % ± 25 % and −20 % ± 18 % for SCdry and ACdry, respectively. The larger underestimate of SCdry than ACdry suggests the models will simulate an aerosol single scattering albedo that is too low. The larger underestimate of SCdry than ambient air AOD is consistent with recent findings that models overestimate scattering enhancement due to hygroscopic growth. The broadly consistent negative bias in AOD and surface scattering suggests an underestimate of aerosol radiative effects in current global aerosol models. Considerable inter-model diversity in the simulated optical properties is often found in regions that are, unfortunately, not or only sparsely covered by ground-based observations. This includes, for instance, the Sahara, Amazonia, central Australia, and the South Pacific. This highlights the need for a better site coverage in the observations, which would enable us to better assess the models, but also the performance of satellite products in these regions. Using fine-mode AOD as a proxy for present-day aerosol forcing estimates, our results suggest that models underestimate aerosol forcing by ca. −15 %, however, with a considerably large interquartile range, suggesting a spread between −35 % and +10 %.

space-based remote sensing↗

Identification of Absorbing Aerosol Types at a Site in the Northern Edge of Indo-Gangetic Plain and a Polluted Valley in the Foothills of the Central Himalayas

Identification of atmospheric aerosol types and characterization of absorbing aerosols, based on AErosol RObotic NETwork (AERONET) data collected during 2013–2014 over two sites in Nepal: Lumbini in the northernmost part of central Indo-Gangetic Plain (IGP) and Kathmandu Valley in foothills of the central Himalayas, have been conducted in the present study. The relationship between four aerosol parameters; Extinction Angstrom Exponent (EAE), Absorption Angstrom Exponent (AAE), Single Scattering Albedo (SSA) and Real Refractive Index (RRI) was analyzed to study the aerosol types. This resulted in the identification of two types of aerosols concerning their origin: biomass burning and urban/industrial mix. Furthermore, to understand the absorbing aerosol types, the relationship between aerosol size parameters; Fine Mode Fraction (FMF) and Angstrom Exponent (AE), and aerosol absorption characteristics; SSA and AAE were investigated. In regards to the absorbing aerosol types, ‘Mostly BC’ was the dominant absorbing aerosol, over both sites, with comparatively negligible contribution from other absorbing aerosol types such as dust. The aerosol subtypes obtained from satellite-borne CALIPSO instrument supported the results derived from the AERONET data. The CALIPSO images also indicated that the aerosols over the foothills of the Himalayas could extend to the height of >5 km above the ground, which could be transported towards the Himalayan and Tibetan Plateau (HTP) region with sensitive ecosystems. The multi-sites based study of long-term records is required to elucidate the nature and trends of aerosols in the HTP region and any perturbation to the atmospheric environment and other environments in this region.

Aerosol types↗

Characterization of Aerosol Episodes in the Greater Mediterranean Sea Area from Satellite Observations (2000-2007)

An algorithm able to identify and characterize episodes of different aerosol types above sea surfaces of the greater Mediterranean basin (GMB), including the Black Sea and the Atlantic Ocean off the coasts of Iberia and northwest Africa, is presented in this study. Based on this algorithm, five types of intense (strong and extreme) aerosol episodes in the GMB are identified and characterized using daily aerosol optical properties from satellite measurements, namely MODIS-Terra, Earth Probe (EP)-TOMS and OMIAura. These aerosol episodes are: (i) biomass-burning/urban-industrial (BU), (ii) desert dust (DD), (iii) dust/sea-salt (DSS), (iv) mixed (MX) and (v) undetermined (UN). The identification and characterization is made with our algorithm using a variety of aerosol properties, namely aerosol optical depth (AOD), Angstrom exponent (a), fine fraction (FF), effective radius (reff) and Aerosol Index (AI). During the study period (2000e2007), the most frequent aerosol episodes are DD, observed primarily in the western and central Mediterranean Sea, and off the northern African coasts, 7 times/year for strong episodes and 4 times/year for extreme ones, on average. The DD episodes yield 40% of all types of strong aerosol episodes in the study region, while they account for 71.5% of all extreme episodes. The frequency of occurrence of strong episodes exhibits specific geographical patterns, for example the BU are mostly observed along the coasts of southern Europe and off the Atlantic coasts of Portugal, the MX episodes off the Spanish Mediterranean coast and over the Adriatic and northern Aegean Sea, while the DSS ones over the western and central Mediterranean Sea. On the other hand, the extreme episodes for all but DD aerosol display more patchy spatial patterns. The strong episodes exhibit AOD at 550 nm as high as 1.6 in the southernmost parts of central and eastern Mediterranean Sea, which rise up to 5 for the extreme, mainly DD and DSS, episodes. Although more than 90% of all aerosol episodes last 1 day, there are few cases, mainly extreme DD episodes, which last up to 4 days. Independently of their type, the Mediterranean aerosol episodes occur more frequently in spring (strong and extreme episodes) and summer (strong episodes) and most rarely during winter. A significant year by year variability of Mediterranean aerosol episodes has been identified, more in terms of their frequency than intensity. An analysis of 5-day back trajectories for the most extreme episodes provides confidence on the obtained results of the algorithm, based on the revealed origin and track of air masses causing the episodes. The 25 and 6% of all strong and extreme episodes, respectively, are MX, thus highlighting the co-existence of different aerosol types in the greater Mediterranean. The intensity of both MX and DSS episodes exhibits similar patterns to those of DD strong ones, indicating that desert dust is a determinant factor for the intensity of aerosol episodes in the Mediterranean, including DSS and MX episodes.

Atmospheric Chemistry↗

Aerosol Retrievals Using Channel 1 and 2 AVHRR Data

The effect of tropospheric aerosols on global climate via the direct and indirect radiative forcings is one of the largest remaining uncertainties in climate change studies. Current assessments of the direct aerosol radiative effect mainly focus on sulfate aerosols. It has become clear, however, that other aerosol types like soil dust and smoke from biomass burning are also likely to be important climate forcing factors. The magnitude and even the sign of the climate forcing caused by these aerosol types is still unknown. General circulation models (GCMs) can be used to estimate the climatic effect of the direct radiative forcing by tropospheric and stratospheric aerosols. Aerosol optical properties are already parameterized in the Goddard Institute for Space Studies GCM. Once the global distribution of aerosol properties (optical thickness, size distribution, and chemical composition) is available, the calculation of the direct aerosol forcing is rather straighfforward. However, estimates of the indirect aerosol effect require additional knowledge of the physics and chemistry of aerosol-cloud interactions which are still poorly understood. One of the main objectives of the Global Aerosol Climatology Project, established in 1998 as a joint initiative of NASA's Radiation Science Program and GEWEX, is to infer the global distribution of aerosols, their properties, and their seasonal and interannual variations for the full period of available satellite data. This will be accomplished primarily through a systematic application of multichannel aerosol retrieval algorithms to existing satellite data and advanced 3-dimensional aerosol chemistry/transport models. In this paper we outline the methodology of analyzing channel 1 and 2 AVHRR radiance data over the oceans and describe preliminary retrieval results.

Mishchenko, Michael I.↗