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Identifying Aerosol Type/Mixture from Aerosol Absorption Properties Using AERONET

Aerosols are generated in the atmosphere through anthropogenic and natural mechanisms. These sources have signatures in the aerosol optical and microphysical properties that can be used to identify the aerosol type/mixture. Spectral aerosol absorption information (absorption Angstrom exponent; AAE) used in conjunction with the particle size parameterization (extinction Angstrom exponent; EAE) can only identify the dominant absorbing aerosol type in the sample volume (e.g., black carbon vs. iron oxides in dust). This AAE/EAE relationship can be expanded to also identify non-absorbing aerosol types/mixtures by applying an absorption weighting. This new relationship provides improved aerosol type distinction when the magnitude of absorption is not equal (e.g, black carbon vs. sulfates). The Aerosol Robotic Network (AERONET) data provide spectral aerosol optical depth and single scattering albedo - key parameters used to determine EAE and AAE. The proposed aerosol type/mixture relationship is demonstrated using the long-term data archive acquired at AERONET sites within various source regions. The preliminary analysis has found that dust, sulfate, organic carbon, and black carbon aerosol types/mixtures can be determined from this AAE/EAE relationship when applying the absorption weighting for each available wavelength (Le., 440, 675, 870nm). Large, non-spherical dust particles absorb in the shorter wavelengths and the application of 440nm wavelength absorption weighting produced the best particle type definition. Sulfate particles scatter light efficiently and organic carbon particles are small near the source and aggregate over time to form larger less absorbing particles. Both sulfates and organic carbon showed generally better definition using the 870nm wavelength absorption weighting. Black carbon generation results from varying combustion rates from a number of sources including industrial processes and biomass burning. Cases with primarily black carbon showed improved definition in the 870nm wavelength absorption weighting due to the increased absorption in the near-infrared wavelengths, while the 440nm wavelength provided better definition when black carbon mixed with dust. Utilization of this particle type scheme provides necessary information for remote sensing applications, which needs a priori knowledge of aerosol type to model the retrieved properties especially over semi-bright surfaces. In fact, this analysis reveals that the aerosol types occurred in mixtures with varying magnitudes of absorption and requires the use of more than one assumed aerosol mixture model. Furthermore, this technique will provide the aerosol transport model community a data set for validating aerosol type.

Giles, D. M.↗

Retrieving Aerosol in a Cloudy Environment: Aerosol Availability as a Function of Spatial and Temporal Resolution

The challenge of using satellite observations to retrieve aerosol properties in a cloudy environment is to prevent contamination of the aerosol signal from clouds, while maintaining sufficient aerosol product yield to satisfy specific applications. We investigate aerosol retrieval availability at different instrument pixel resolutions, using the standard MODIS aerosol cloud mask applied to MODIS data and a new GOES-R cloud mask applied to GOES data for a domain covering North America and surrounding oceans. Aerosol availability is not the same as the cloud free fraction and takes into account the technqiues used in the MODIS algorithm to avoid clouds, reduce noise and maintain sufficient numbers of aerosol retrievals. The inherent spatial resolution of each instrument, 0.5x0.5 km for MODIS and 1x1 km for GOES, is systematically degraded to 1x1 km, 2x2 km, 4x4 km and 8x8 km resolutions and then analyzed as to how that degradation would affect the availability of an aerosol retrieval, assuming an aerosol product resolution at 8x8 km. The results show that as pixel size increases, availability decreases until at 8x8 km 70% to 85% of the retrievals available at 0.5 km have been lost. The diurnal pattern of aerosol retrieval availability examined for one day in the summer suggests that coarse resolution sensors (i.e., 4x4 km or 8x8 km) may be able to retrieve aerosol early in the morning that would otherwise be missed at the time of current polar orbiting satellites, but not the diurnal aerosol properties due to cloud cover developed during the day. In contrast finer resolution sensors (i.e., 1x1 km or 2x2 km) have much better opportunity to retrieve aerosols in the partly cloudy scenes and better chance of returning the diurnal aerosol properties. Large differences in the results of the two cloud masks designed for MODIS aerosol and GOES cloud products strongly reinforce that cloud masks must be developed with specific purposes in mind and that a generic cloud mask applied to an independent aerosol retrieval will likely fail.

Remer, Lorraine A.↗

Investigating Aerosol and Meteorological Influences on Convective Clouds in Houston, Texas, during the TRACER/ESCAPE Field Campaigns

Aerosols serve as cloud condensation nuclei, shaping the microphysical properties of cloud droplets. Aerosol effects on convective clouds are complex and remain controversial. The debate centers around the process of aerosol-induced invigoration of deep convection, a phenomenon that could significantly affect convective cloud properties but lacks robust evidence due to methodological limitations in observational approaches and questions about the robustness of modeling studies. Resolving these discrepancies is crucial for understanding how aerosols affect the atmosphere. Here, this study examines the effects of meteorological and aerosol parameters in a weakly synoptic-driven convective environment, where the influence of aerosols may be more pronounced and observable. Daily atmospheric soundings and aerosol concentrations from several ground instruments collected during the summer of 2022 in Houston, Texas, as part of the Tracking Aerosol Convection interactions Experiment (TRACER) and Experiment of Sea Breeze Convection, Aerosols, Precipitation, and Environment (ESCAPE) field campaigns are analyzed. Statistical learning methods are applied to uncover the complex relationships between aerosols, meteorology, and convective cloud characteristics, such as cell area and echo-top height. The findings reveal that higher aerosol concentrations are associated with narrower convective cells, which we argue contradicts the idea of stronger convection with increased aerosol loading. However, once the data are clustered by the synoptic environment, the relationship between aerosol loading and convective cell area diminishes, indicating that the covariablity between synoptic-scale weather patterns, local thermodynamics, and aerosol loading makes it challenging to draw definitive conclusions about the specific impacts of aerosols on convective cloud properties.

54 ENVIRONMENTAL SCIENCES↗

Impacts of aerosol size-dependent below-cloud scavenging on tropospheric aerosol in the NASA GEOS model

Wet deposition is the major sink for a suite of tropospheric aerosols, and thus largely affects the global distribution and lifetime of aerosols as well as the formation of clouds in the atmosphere. In this study, we implement the aerosol size-dependent below-cloud scavenging (BCS; washout) parameterization of Croft et al. (Atmos. Chem. Phys., 2009; hereafter referred to as C09) in the GOCART bulk aerosol scheme coupled with the NASA Goddard Earth Observing System (GEOS) model, and evaluate the simulated tropospheric aerosols against surface, airborne, and satellite observations. The current below-cloud scavenging in GOCART employs a first-order removal function with a constant scavenging coefficient that is independent of aerosol sizes and precipitation fluxes. The C09 BCS parameterization instead calculates aerosol below-cloud scavenging coefficients based on a size-dependent collision efficiency between aerosol particles and raindrops (or snow crystals). A look-up table of compiled collision efficiencies provides scavenging coefficients for sixty aerosol sizes and nine rain flux rates. We determine instantaneous coefficients according to the C09 BCS look-up table, precipitation fluxes, and a log-normal size distribution of aerosols. The implemented BCS parameterization tends to result in a large diversity of scavenging coefficient values with higher magnitudes, leading to more efficient scavenging. The model-simulated global mean tropospheric Pb-210 aerosol lifetime decreases from 7.4 days to 5.8 days. The separate consideration of rain and snow conditions in the scavenging coefficient lookup table leads to a bi-mode distribution of scavenging coefficients. These changes also cause increased mass fractions of smaller aerosols compared to the current simulation. We examine the impacts of the C09 BCS parameterization on the simulated aerosol vertical profiles, tropospheric lifetimes, and deposition fluxes through comparisons with NASA aircraft measurements (ATom), surface observations of aerosol concentrations (IMPROVE) and wet deposition fluxes (NADP and APQMP), and MODIS aerosol optical depth (AOD) retrievals.

Aerosols↗

The significant impact of aerosol vertical structure on lower atmosphere stability and its critical role in aerosol–planetary boundary layer (PBL) interactions

The aerosol–planetary boundary layer (PBL) interaction was proposed as an important mechanism to stabilize the atmosphere and exacerbate surface air pollution. Despite the tremendous progress made in understanding this process, its magnitude and significance still have large uncertainties and vary largely with aerosol distribution and meteorological conditions. In this study, we focus on the role of aerosol vertical distribution in thermodynamic stability and PBL development by jointly using micropulse lidar, sun photometer, and radiosonde measurements taken in Beijing. Despite the complexity of aerosol vertical distributions, cloud-free aerosol structures can be largely classified into three types: well-mixed, decreasing with height, and inverse structures. The aerosol–PBL relationship and diurnal cycles of the PBL height and PM 2.5 associated with these different aerosol vertical structures show distinct characteristics. The vertical distribution of aerosol radiative forcing differs drastically among the three types, with strong heating in the lower, middle, and upper PBL, respectively. Such a discrepancy in the heating rate affects the atmospheric buoyancy and stability differently in the three distinct aerosol structures. Absorbing aerosols have a weaker effect of stabilizing the lower atmosphere under the decreasing structure than under the inverse structure. As a result, the aerosol–PBL interaction can be strengthened by the inverse aerosol structure and can be potentially neutralized by the decreasing structure. Moreover, aerosols can both enhance and suppress PBL stability, leading to both positive and negative feedback loops. This study attempts to improve our understanding of the aerosol–PBL interaction, showing the importance of the observational constraint of aerosol vertical distribution for simulating this interaction and consequent feedbacks.

54 ENVIRONMENTAL SCIENCES↗

Modeled and observed properties related to the direct aerosol radiative effect of biomass burning aerosol over the southeastern Atlantic

Biomass burning smoke is advected over the southeastern Atlantic Ocean between July and October of each year. This smoke plume overlies and mixes into a region of persistent low marine clouds. Model calculations of climate forcing by this plume vary significantly in both magnitude and sign. NASA EVS-2 (Earth Venture Suborbital-2) ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) had deployments for field campaigns off the west coast of Africa in 3 consecutive years (September 2016, August 2017, and October 2018) with the goal of better characterizing this plume as a function of the monthly evolution by measuring the parameters necessary to calculate the direct aerosol radiative effect. Here, this dataset and satellite retrievals of cloud properties are used to test the representation of the smoke plume and the underlying cloud layer in two regional models (WRF-CAM5 and CNRM-ALADIN) and two global models (GEOS and UM-UKCA). The focus is on the comparisons of those aerosol and cloud properties that are the primary determinants of the direct aerosol radiative effect and on the vertical distribution of the plume and its properties. The representativeness of the observations to monthly averages are tested for each field campaign, with the sampled mean aerosol light extinction generally found to be within 20 % of the monthly mean at plume altitudes. When compared to the observations, in all models, the simulated plume is too vertically diffuse and has smaller vertical gradients, and in two of the models (GEOS and UM-UKCA), the plume core is displaced lower than in the observations. Plume carbon monoxide, black carbon, and organic aerosol masses indicate underestimates in modeled plume concentrations, leading, in general, to underestimates in mid-visible aerosol extinction and optical depth. Biases in mid-visible single scatter albedo are both positive and negative across the models. Observed vertical gradients in single scatter albedo are not captured by the models, but the models do capture the coarse temporal evolution, correctly simulating higher values in October (2018) than in August (2017) and September (2016). Uncertainties in the measured absorption Ångstrom exponent were large but propagate into a negligible (<4 %) uncertainty in integrated solar absorption by the aerosol and, therefore, in the aerosol direct radiative effect. Model biases in cloud fraction, and, therefore, the scene albedo below the plume, vary significantly across the four models. The optical thickness of clouds is, on average, well simulated in the WRF-CAM5 and ALADIN models in the stratocumulus region and is underestimated in the GEOS model; UM-UKCA simulates cloud optical thickness that is significantly too high. Overall, the study demonstrates the utility of repeated, semi-random sampling across multiple years that can give insights into model biases and how these biases affect modeled climate forcing. The combined impact of these aerosol and cloud biases on the direct aerosol radiative effect (DARE) is estimated using a first-order approximation for a subset of five comparison grid boxes. A significant finding is that the observed grid box average aerosol and cloud properties yield a positive (warming) aerosol direct radiative effect for all five grid boxes, whereas DARE using the grid-box-averaged modeled properties ranges from much larger positive values to small, negative values. It is shown quantitatively how model biases can offset each other, so that model improvements that reduce biases in only one property (e.g., single scatter albedo but not cloud fraction) would lead to even greater biases in DARE. Across the models, biases in aerosol extinction and in cloud fraction and optical depth contribute the largest biases in DARE, with aerosol single scatter albedo also making a significant contribution.

54 ENVIRONMENTAL SCIENCES↗

Strategy to use the Terra Aerosol Information to Derive the Global Aerosol Radiative Forcing of Climate

Terra will derive the aerosol optical thickness and properties. The aerosol properties can be used to distinguish between natural and human-made aerosol. In the polar orbit Terra will measure aerosol only once a day, around 10:30 am. How will we use this information to study the global radiative impacts of aerosol on climate? We shall present a strategy to address this problem. It includes the following steps: - From the Terra aerosol optical thickness and size distribution model we derive the effect of aerosol on reflection of solar radiation at the top of the atmosphere. In a sensitivity study we show that the effect of aerosol on solar fluxes can be derived 10 times more accurately from the MODIS data than derivation of the optical thickness itself. Applications to data over several regions will be given. - Using 1/2 million AERONET global data of aerosol spectral optical thickness we show that the aerosol optical thickness and properties during the Terra 10:30 pass are equivalent to the daily average. Due to the aerosol lifetime of several days measurements at this time of the day are enough to assess the daily impact of aerosol on radiation. - Aerosol impact on the top of the atmosphere is only part of the climate question. The INDOEX experiment showed that addressing the impact of aerosol on climate, requires also measurements of the aerosol forcing at the surface. This can be done by a combination of measurements of MODIS and AERONET data.

Kaufman, Yoram J.↗

Identifying Chemical Aerosol Signatures Using Optical Suborbital Observations: How Much Can Optical Properties Tell us about Aerosol Composition?

Improvements in air quality and Earth’s climate predictions require improvements of the aerosol speciation in chemical transport models, using observational constraints. Aerosol speciation (e.g., organic aerosols, black carbon, sulfate, nitrate, ammonium, dust or sea salt) is typically determined using in situ instrumentation. Continuous, routine surface network aerosol composition measurements are not uniformly widespread over the globe. Satellites, on the other hand, can provide a maximum coverage of the horizontal and vertical atmosphere but observe aerosol optical properties (and not aerosol speciation) based on remote sensing instrumentation. Combinations of satellite-derived aerosol optical properties can inform on air mass aerosol types (AMTs e.g., clean marine, dust, polluted continental). However, these AMTs are subjectively defined, might often be misclassified and are hard to relate to the critical parameters that need to be refined in models. In this paper, we derive AMTs that are more directly related to sources and hence to speciation. They are defined, characterized, and derived using simultaneous in situ gas-phase, chemical and optical instruments on the same aircraft during the Study of Emissions and Atmospheric Composition, Clouds, and Climate Coupling by Regional Surveys (SEAC4RS, US, summer of 2013). First, we prescribe well-informed AMTs that display distinct aerosol chemical and optical signatures to act as a training AMT dataset. These in situ observations reduce the errors and ambiguities in the selection of the AMT training dataset. We also investigate the relative skill of various combinations of aerosol optical properties to define AMTs and how much these optical properties can capture dominant aerosol speciation. We find distinct optical signatures for biomass burning (from agricultural or wildfires), biogenic and dust-influence AMTs. Useful aerosol optical properties to characterize these signatures are the extinction angstrom exponent (EAE), the single scattering albedo, the difference of single scattering albedo in two wavelengths, the absorption coefficient, the absorption angstrom exponent (AAE), and the real part of the refractive index (RRI). We find that all four AMTs studied when prescribed using mostly airborne in situ gas measurements, can be successfully extracted from at least three combinations of airborne in situ aerosol optical properties (e.g., EAE, AAE and RRI) over the US during SEAC4RS. However, we find that the optically based classifications for BB from agricultural fires and polluted dust include a large percentage of misclassifications that limit the usefulness of results relating to those classes. The technique and results presented in this study are suitable to develop a representative, robust and diverse source-based AMT database. This database could then be used for widespread retrievals of AMTs using existing and future remote sensing suborbital instruments/networks. Ultimately, it has the potential to provide a much broader observational aerosol data set to evaluate chemical transport and air quality models than is currently available by direct in situ measurements. This study illustrates how essential it is to explore existing airborne datasets to bridge chemical and optical signatures of different AMTs, before the implementation of future spaceborne missions (e.g., the next generation of Earth Observing System (EOS) satellites addressing Aerosol, Cloud, Convection and Precipitation (ACCP) designated observables).

Meloe S F Kacenelenbogen↗

Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA)

With their extensive coverage, marine low clouds greatly impact global climate. Presently, marine low clouds are poorly represented in global climate models, and the response of marine low clouds to changes in atmospheric greenhouse gases and aerosols remains the major source of uncertainty in climate simulations. The Eastern North Atlantic (ENA) is a region of persistent but diverse subtropical marine boundary layer clouds, whose albedo and precipitation are highly susceptible to perturbations in aerosol properties. In addition, the ENA is periodically impacted by continental aerosols, making it an excellent location to study the cloud condensation nuclei (CCN) budget in a remote marine region periodically perturbed by anthropogenic emissions, and to investigate the impacts of long-range transport of aerosols on remote marine clouds. The Aerosol and Cloud Experiments in Eastern North Atlantic (ACE-ENA) campaign was motivated by the need of comprehensive in-situ measurements for improving the understanding of marine boundary layer CCN budget, cloud and drizzle microphysics, and the impact of aerosol on marine low cloud and precipitation. The airborne deployments took place from June 21 to July 20, 2017 and January 15 to February 18, 2018 in the Azores. The flights were designed to maximize the synergy between in-situ airborne measurements and ongoing long-term observations at a ground site. Here we present measurements, observation strategy, meteorological conditions during the campaign, and preliminary findings. Lastly, we discuss future analyses and modeling studies that improve the understanding and representation of marine boundary layer aerosols, clouds, precipitation, and the interactions among them.

54 ENVIRONMENTAL SCIENCES↗

Multi-Sensor Cloud and Aerosol Retrieval Simulator and Remote Sensing from Model Parameters : Aerosols - Part 2

The Multi-sensor Cloud Retrieval Simulator (MCRS) produces a simulated radiance product from any high-resolution general circulation model with interactive aerosol as if a specific sensor such as the Moderate Resolution Imaging Spectroradiometer (MODIS) were viewing a combination of the atmospheric column and land ocean surface at a specific location. Previously the MCRS code only included contributions from atmosphere and clouds in its radiance calculations and did not incorporate properties of aerosols. In this paper we added a new aerosol properties module to the MCRS code that allows users to insert a mixture of up to 15 different aerosol species in any of 36 vertical layers. This new MCRS code is now known as MCARS (Multi-sensor Cloud and Aerosol Retrieval Simulator). Inclusion of an aerosol module into MCARS not only allows for extensive, tightly controlled testing of various aspects of satellite operational cloud and aerosol properties retrieval algorithms, but also provides a platform for comparing cloud and aerosol models against satellite measurements. This kind of two-way platform can improve the efficacy of model parameterizations of measured satellite radiances, allowing the assessment of model skill consistently with the retrieval algorithm. The MCARS code provides dynamic controls for appearance of cloud and aerosol layers. Thereby detailed quantitative studies of the impacts of various atmospheric components can be controlled. In this paper we illustrate the operation of MCARS by deriving simulated radiances from various data field output by the Goddard Earth Observing System version 5 (GEOS-5) model. The model aerosol fields are prepared for translation to simulated radiance using the same model sub grid variability parameterizations as are used for cloud and atmospheric properties profiles, namely the ICA technique. After MCARS computes modeled sensor radiances equivalent to their observed counterparts, these radiances are presented as input to operational remote-sensing algorithms. Specifically, the MCARS-computed radiances are input into the processing chain used to produce the MODIS Data Collection 6 aerosol product (MOYD04). TheMOYD04 product is of course normally produced from MOYD021KM MODIS Level-1B radiance product directly acquired by the MODIS instrument. MCARS matches the format and metadata of a MOYD021KM product. The resulting MCARS output can be directly provided to MODAPS (MODIS Adaptive Processing System) as input to various operational atmospheric retrieval algorithms. Thus the operational algorithms can be tested directly without needing to make any software changes to accommodate an alternative input source. We show direct application of this synthetic product in analysis of the performance of the MOD04 operational algorithm. We use biomass-burning case studies over Amazonia employed in a recent Working Group on Numerical Experimentation (WGNE)-sponsored study of aerosol impacts on numerical weather prediction (Freitas et al., 2015). We demonstrate that a known low bias in retrieved MODIS aerosol optical depth appears to be due to a disconnect between actual column relative humidity and the value assumed by the MODIS aerosol product.

aerosol retrieval↗

Towards a Global Aerosol Climatology: Preliminary Trends in Tropospheric Aerosol Amounts and Corresponding Impact on Radiative Forcing between 1950 and 1990

A global aerosol climatology is needed in the study of decadal temperature change due to natural and anthropogenic forcing of global climate change. A preliminary aerosol climatology has been developed from global transport models for a mixture of sulfate and carbonaceous aerosols from fossil fuel burning, including also contributions from other major aerosol types such as soil dust and sea salt. The aerosol distributions change for the period of 1950 to 1990 due to changes in emissions of SO2 and carbon particles from fossil fuel burning. The optical thickness of fossil fuel derived aerosols increased by nearly a factor of 3 during this period, with particularly strong increase in eastern Asia over the whole time period. In countries where environmental laws came into effect since the early 1980s (e.g. US and western Europe), emissions and consequently aerosol optical thicknesses did not increase considerably after 1980, resulting in a shift in the global distribution pattern over this period. In addition to the optical thickness, aerosol single scattering albedos may have changed during this period due to different trends in absorbing black carbon and reflecting sulfate aerosols. However, due to the uncertainties in the emission trends, this change cannot be determined with any confidence. Radiative forcing of this aerosol distribution is calculated for several scenarios, resulting in a wide range of uncertainties for top-of-atmosphere (TOA) forcings. Uncertainties in the contribution of the strongly absorbing black carbon aerosol leads to a range in TOA forcings of ca. -0.5 to + 0.1 Wm (exp. -2), while the change in aerosol distributions between 1950 to 1990 leads to a change of -0.1 to -0.3 Wm (exp. -2), for fossil fuel derived aerosol with a "moderate" contribution of black carbon aerosol.

Tegen, Ina↗

MODIS Observation of Aerosols over Southern Africa During SAFARI 2000: Data, Validation, and Estimation of Aerosol Radiative Forcing

Aerosol properties, including optical thickness and size parameters, are retrieved operationally from the MODIS sensor onboard the Terra satellite launched on 18 December 1999. The predominant aerosol type over the Southern African region is smoke, which is generated from biomass burning on land and transported over the southern Atlantic Ocean. The SAFARI-2000 period experienced smoke aerosol emissions from the regular biomass burning activities as well as from the prescribed burns administered on the auspices of the experiment. The MODIS Aerosol Science Team (MAST) formulates and implements strategies for the retrieval of aerosol products from MODIS, as well as for validating and analyzing them in order to estimate aerosol effects in the radiative forcing of climate as accurately as possible. These activities are carried out not only from a global perspective, but also with a focus on specific regions identified as having interesting characteristics, such as the biomass burning phenomenon in southern Africa and the associated smoke aerosol, particulate, and trace gas emissions. Indeed, the SAFARI-2000 aerosol measurements from the ground and from aircraft, along with MODIS, provide excellent data sources for a more intensive validation and a closer study of the aerosol characteristics over Southern Africa. The SAFARI-2000 ground-based measurements of aerosol optical thickness (AOT) from both the automatic Aerosol Robotic Network (AERONET) and handheld Sun photometers have been used to validate MODIS retrievals, based on a sophisticated spatio-temporal technique. The average global monthly distribution of aerosol from MODIS has been combined with other data to calculate the southern African aerosol daily averaged (24 hr) radiative forcing over the ocean for September 2000. It is estimated that on the average, for cloud free conditions over an area of 9 million square kin, this predominantly smoke aerosol exerts a forcing of -30 W/square m C lose to the terrestrial surface and -10 W/square m at the top of the atmosphere (TOA). While cooling the surface and Earth system, the difference of 20 W/square m is energy that heats the atmosphere.

Ichoku, Charles↗

Global Aerosol Optical Models and Lookup Tables for the New MODIS Aerosol Retrieval over Land

Since 2000, MODIS has been deriving aerosol properties over land from MODIS observed spectral reflectance, by matching the observed reflectance with that simulated for selected aerosol optical models, aerosol loadings, wavelengths and geometrical conditions (that are contained in a lookup table or 'LUT'). Validation exercises have showed that MODIS tends to under-predict aerosol optical depth (tau) in cases of large tau (tau greater than 1.0), signaling errors in the assumed aerosol optical properties. Using the climatology of almucantur retrievals from the hundreds of global AERONET sunphotometer sites, we found that three spherical-derived models (describing fine-sized dominated aerosol), and one spheroid-derived model (describing coarse-sized dominated aerosol, presumably dust) generally described the range of observed global aerosol properties. The fine dominated models were separated mainly by their single scattering albedo (omega(sub 0)), ranging from non-absorbing aerosol (omega(sub 0) approx. 0.95) in developed urban/industrial regions, to neutrally absorbing aerosol (omega(sub 0) approx.90) in forest fire burning and developing industrial regions, to absorbing aerosol (omega(sub 0) approx. 0.85) in regions of savanna/grassland burning. We determined the dominant model type in each region and season, to create a 1 deg. x 1 deg. grid of assumed aerosol type. We used vector radiative transfer code to create a new LUT, simulating the four aerosol models, in four MODIS channels. Independent AERONET observations of spectral tau agree with the new models, indicating that the new models are suitable for use by the MODIS aerosol retrieval.

Levy, Robert C.↗

Estimating Marine Aerosol Particle Volume and Number from Maritime Aerosol Network Data

As well as spectral aerosol optical depth (AOD), aerosol composition and concentration (number, volume, or mass) are of interest for a variety of applications. However, remote sensing of these quantities is more difficult than for AOD, as it is more sensitive to assumptions relating to aerosol composition. This study uses spectral AOD measured on Maritime Aerosol Network (MAN) cruises, with the additional constraint of a microphysical model for unpolluted maritime aerosol based on analysis of Aerosol Robotic Network (AERONET) inversions, to estimate these quantities over open ocean. When the MAN data are subset to those likely to be comprised of maritime aerosol, number and volume concentrations obtained are physically reasonable. Attempts to estimate surface concentration from columnar abundance, however, are shown to be limited by uncertainties in vertical distribution. Columnar AOD at 550 nm and aerosol number for unpolluted maritime cases are also compared with Moderate Resolution Imaging Spectroradiometer (MODIS) data, for both the present Collection 5.1 and forthcoming Collection 6. MODIS provides a best-fitting retrieval solution, as well as the average for several different solutions, with different aerosol microphysical models. The average solution MODIS dataset agrees more closely with MAN than the best solution dataset. Terra tends to retrieve lower aerosol number than MAN, and Aqua higher, linked with differences in the aerosol models commonly chosen. Collection 6 AOD is likely to agree more closely with MAN over open ocean than Collection 5.1. In situations where spectral AOD is measured accurately, and aerosol microphysical properties are reasonably well-constrained, estimates of aerosol number and volume using MAN or similar data would provide for a greater variety of potential comparisons with aerosol properties derived from satellite or chemistry transport model data.

Sayer, A. M.↗

The Role of Cloud Contamination, Aerosol Layer Height and Aerosol Model in the Assessment of the OMI Near-UV Retrievals Over the Ocean

Retrievals of aerosol optical depth (AOD) at 388 nm over the ocean from the Ozone Monitoring Instrument (OMI) two-channel near-UV algorithm (OMAERUV) have been compared with independent AOD measurements. The analysis was carried out over the open ocean (OMI and MODerate-resolution Imaging Spectrometer (MODIS) AOD comparisons) and over coastal and island sites (OMI and AERONET, the AErosol RObotic NETwork). Additionally, a research version of the retrieval algorithm (using MODIS and CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) information as constraints) was utilized to evaluate the sensitivity of the retrieval to different assumed aerosol properties. Overall, the comparison resulted in differences (OMI minus independent measurements) within the expected levels of uncertainty for the OMI AOD retrievals (0.1 for AOD less than 0.3, 30% for AOD greater than 0.3). Using examples from case studies with outliers, the reasons that led to the observed differences were examined with specific purpose to determine whether they are related to instrument limitations (i.e., pixel size, calibration) or algorithm assumptions (such as aerosol shape, aerosol height). The analysis confirms that OMAERUV does an adequate job at rejecting cloudy scenes within the instrument's capabilities. There is a residual cloud contamination in OMI pixels with quality flag 0 (the best conditions for aerosol retrieval according to the algorithm), resulting in a bias towards high AODs in OMAERUV. This bias is more pronounced at low concentrations of absorbing aerosols (AOD 388 nm approximately less than 0.5). For higher aerosol loadings, the bias remains within OMI's AOD uncertainties. In pixels where OMAERUV assigned a dust aerosol model, a fraction of them (less than 20 %) had retrieved AODs significantly lower than AERONET and MODIS AODs. In a case study, a detailed examination of the aerosol height from CALIOP and the AODs from MODIS, along with sensitivity tests, was carried out by varying the different assumed parameters in the retrieval (imaginary index of refraction, size distribution, aerosol height, particle shape). It was found that the spherical shape assumption for dust in the current retrieval is the main cause of the underestimate. In addition, it is demonstrated in an example how an incorrect assumption of the aerosol height can lead to an underestimate. Nevertheless, this is not as significant as the effect of particle shape. These findings will be incorporated in a future version of the retrieval algorithm.

aerosols↗

Use of A-Train Aerosol Observations to Constrain Direct Aerosol Radiative Effects (DARE) Comparisons with Aerocom Models and Uncertainty Assessments

We describe a technique for combining multiple A-Train aerosol data sets, namely MODIS spectral AOD (aerosol optical depth), OMI AAOD (absorption aerosol optical depth) and CALIOP aerosol backscatter retrievals (hereafter referred to as MOC retrievals) to estimate full spectral sets of aerosol radiative properties, and ultimately to calculate the 3-D distribution of direct aerosol radiative effects (DARE). We present MOC results using almost two years of data collected in 2007 and 2008, and show comparisons of the aerosol radiative property estimates to collocated AERONET retrievals. Use of the MODIS Collection 6 AOD data derived with the dark target and deep blue algorithms has extended the coverage of the MOC retrievals towards higher latitudes. The MOC aerosol retrievals agree better with AERONET in terms of the single scattering albedo (ssa) at 441 nm than ssa calculated from OMI and MODIS data alone, indicating that CALIOP aerosol backscatter data contains information on aerosol absorption. We compare the spatio-temporal distribution of the MOC retrievals and MOC-based calculations of seasonal clear-sky DARE to values derived from four models that participated in the Phase II AeroCom model intercomparison initiative. Overall, the MOC-based calculations of clear-sky DARE at TOA over land are smaller (less negative) than previous model or observational estimates due to the inclusion of more absorbing aerosol retrievals over brighter surfaces, not previously available for observationally-based estimates of DARE. MOC-based DARE estimates at the surface over land and total (land and ocean) DARE estimates at TOA are in between previous model and observational results. Comparisons of seasonal aerosol property to AeroCom Phase II results show generally good agreement best agreement with forcing results at TOA is found with GMI-MerraV3. We discuss sampling issues that affect the comparisons and the major challenges in extending our clear-sky DARE results to all-sky conditions. We present estimates of clear-sky and all-sky DARE and show uncertainties that stem from the assumptions in the spatial extrapolation and accuracy of aerosol and cloud properties, in the diurnal evolution of these properties, and in the radiative transfer calculations.

aerosol↗

Impacts of aerosol size-dependent below-cloud scavenging on tropospheric aerosol in the NASA GEOS model

Cloud scavenging is the major sink for a suite of tropospheric aerosols, and thus largely affects the global distribution and lifetime of aerosols as well as the formation of clouds. Simplified model parameterizations of cloud scavenging of aerosols substantially contribute to large uncertainties in the simulated aerosol burdens, spatial distributions, lifetimes, as well as aerosol radiative forcing. Here we evaluate the wet scavenging scheme in the current NASA GEOS model, develop more physically-based parameterizations of below-cloud scavenging, and assess the impacts of the new scavenging parameterizations on the GEOS simulations of aerosols. The current below-cloud scavenging (BCS; washout) scheme uses a first-order removal with a constant scavenging coefficient. We replaced the current scheme with a size-dependent parameterization of Croft et al.(Atmos. Chem. Phys., 2009; hereafter referred to as C09). The C09 BCS parameterizations calculate aerosol below-cloud scavenging coefficients based on a size-dependent collision efficiency between aerosol particles and raindrops (or snow crystals). A look-up table of compiled collision efficiencies provides values for sixty aerosol sizes and nine rain flux rates. Snow-aerosol collision efficiencies are a function of the sixty aerosol sizes only. We assume a log-normal size distribution for aerosols (bulk) in GOCART. The collision efficiencies are then calculated online using a bilinear interpolation from the look-up table for the given aerosol sizes and precipitation flux rates in the model.

aerosols↗

Three-Wavelength Approach for Aerosol-Cloud Discrimination in the Sage III/ISS Aerosol Extinction Dataset

The tropical upper troposphere and lower stratosphere (UTLS) region is dominated by aerosols and clouds affecting Earth’s radiation budget and climate. Thus, satellites’ continuous monitoring and identification of these layers is crucial for quantifying their radiative impact. However, distinguishing between aerosols and clouds is challenging, especially under the perturbed UTLS conditions during post-volcanic eruptions and wildfire events. Aerosol-cloud discrimination is primarily based on their disparate wavelength-dependent scattering and absorption properties. In this study, we use aerosol extinction observations in the tropical (15°N-15°S) UTLS from June 2017 to February 2021, available from the latest generation of the Stratospheric Aerosol and Gas Experiment (SAGE) instrument-SAGE III onboard the International Space Station (ISS) to study aerosols and clouds. During this period, the SAGE III/ISS provided better coverage over the tropics at additional wavelength channels (relative to previous SAGE missions) and witnessed several volcanic and wildfire events that perturbed the tropical UTLS. We explore the advantage of having an extinction coefficient at an additional wavelength channel (1550 nm) from the SAGE III/ISS in aerosol-cloud discrimination using a method based on thresholds of two extinction coefficient ratios, R1R1 (520 nm/1020 nm) and R2R2 (1020 nm/1550 nm). This method was proposed earlier by Kent et al. [Appl. Opt. 36, 8639 (1997) [CrossRef] ] for the SAGE III-Meteor-3M but was never tested for the tropical region under volcanically perturbed conditions. We call this method the Extinction Color Ratio (ECR) method. The ECR method is applied to the SAGE III/ISS aerosol extinction data to obtain cloud-filtered aerosol extinction coefficients, cloud-top altitude, and seasonal cloud occurrence frequency during the entire study period. Cloud-filtered aerosol extinction coefficient obtained using the ECR method revealed the presence of enhanced aerosols in the UTLS following volcanic eruptions and wildfire events consistent with the Ozone Mapping and Profiler Suite (OMPS) and space-borne lidar-Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP). The cloud-top altitude obtained from the SAGE III/ISS is within 1 km of the nearly co-located observations from OMPS and CALIOP. In general, the seasonal mean cloud-top altitude from the SAGE III/ISS events peaks during the December, January, and February months, with sunset events showing higher cloud tops than the sunrise events, indicating the seasonal and diurnal variation of the tropical convection. The seasonal altitude distribution of cloud occurrence frequency obtained from the SAGE III/ISS also agrees well with CALIOP observations within 10%. We show that the ECR method is a simple approach that relies on thresholds independent of the sampling period, providing cloud-filtered aerosol extinction coefficients uniformly for climate studies irrespective of the UTLS conditions. However, since the predecessor of SAGE III did not include a 1550 nm channel, the usefulness of this approach is limited to short-term climate studies after 2017.

Clouds Aerosols↗