Global Aerosol System Research Articles

Increasing aerosol optical depth spatial and temporal availability by merging datasets from geostationary and sun-synchronous satellites

Abstract. This comprehensive study analyzed aerosol products from six low-Earth orbit (LEO) and geostationary Earth orbit (GEO) sensors. LEO sensors like the MODerate resolution Imaging Spectroradiometer (MODIS) and VIsible InfraRed Suite (VIIRS) provide one to two daily global measurements, while GEO sensors (Advanced Himawari Imager: AHI, Advanced Baseline Imager: ABI) offer high-frequency data (∼ 10 min) over specific regions. The combination of LEO and GEO capabilities offers expanded coverage of the global aerosol system if aerosol retrievals are applied consistently across all sensors and packaged in an easy-to-use product. The Dark Target aerosol retrieval algorithm was applied to the six sensors, and the resulting Level 2 aerosol optical depth (AOD) products were gridded and merged into a Level 3 quarter-degree latitude–longitude grid with a 30 min temporal resolution, providing the necessary consistency and packaging. Validation of this packaged Level 3 AOD product against Aerosol Robotics NETwork (AERONET) measurements across global locations showcased the merged product's robustness with a correlation coefficient of 0.83, revealing a global mean bias of approximately ±0.05, with 65.5 % of retrievals falling within an expected uncertainty range, underlining the reliability of the dataset. The new gridded Level 3 dataset significantly improved daily global coverage to nearly 45 %, overcoming the limitations of individual sensors, which typically range from 12 % to 25 %. Furthermore, this merged dataset approximates the diurnal cycle of AOD observed by AERONET, thus offering insights into diurnal signatures retrieved elsewhere. The resulting dataset's high spatiotemporal resolution and improved global coverage, especially in regions covered by GEO sensors (Americas and Asia), make it a valuable tool for diverse applications. Tracking aerosol transport from phenomena like wildfires and dust storms is gaining precision, enabling enhanced air quality forecasting and hindcasting. Additionally, the study positions the merged dataset as a significant asset for evaluating and intercomparing regional or global model simulations, which was previously unattainable in such a gridded format. The dataset and fusion framework layout in this study have the potential to include data from recently (future) launched other GEO (FCI, AMI) and LEO (PACE, VIIRS-JPSS) sensors.

Opinion: Aerosol remote sensing over the next 20 years

Abstract. More than 2 decades ago, aerosol remote sensing underwent a revolution with the launch of the Terra and Aqua satellites. Advancement continued via additional launches carrying new passive and active sensors. Capable of retrieving parameters characterizing aerosol loading, rudimentary particle properties and in some cases aerosol layer height, the satellite view of Earth's aerosol system came into focus. The modeling communities have made similar advances. Now the efforts have continued long enough that we can see developing trends in both the remote sensing and modeling communities, allowing us to speculate about the future and how the community will approach aerosol remote sensing 20 years from now. We anticipate technology that will replace today's standard multi-wavelength radiometers with hyperspectral and/or polarimetry, all viewing at multiple angles. These will be supported by advanced active sensors with the ability to measure profiles of aerosol extinction in addition to backscatter. The result will be greater insight into aerosol particle properties. Algorithms will move from being primarily physically based to include an increasing degree of machine-learning methods, but physically based techniques will not go extinct. However, the practice of applying algorithms to a single sensor will be in decline. Retrieval algorithms will encompass multiple sensors and all available ground measurements in a unifying framework, and these inverted products will be ingested directly into assimilation systems, becoming “cyborgs”: half observations, half model. In 20 years we will see a true democratization in space with nations large and small, private organizations, and commercial entities of all sizes launching space sensors. With this increasing number of data and aerosol products available, there will be a lot of bad data. User communities will organize to set standards, and the large national space agencies will lead the effort to maintain quality by deploying and maintaining validation ground networks and focused field experiments. Through it all, interest will remain high in the global aerosol system and how that system affects climate, clouds, precipitation and dynamics, air quality, the environment and public health, transport of pathogens and fertilization of ecosystems, and how these processes are adapting to a changing climate.

Investigating the Spatial and Temporal Limitations for Remote Sensing of Wildfire Smoke Using Satellite and Airborne Imagers During FIREX‐AQ

AbstractStarting from point sources, wildfire smoke is important in the global aerosol system. The ability to characterize smoke near‐source is key to modeling smoke dispersion and predicting air quality. With hemispheric views and 10‐min refresh, imagers in Geostationary (GEO) orbit have advantages monitoring smoke over once‐per‐day sensors in low‐earth orbit (LEO). However, both can be inadequate in capturing the characteristics of smoke plumes close to their sources due to too‐coarse spatial resolution (both detector and product resolution), too‐sparse temporal resolution (from LEO sensors), and too‐conservative masking. In addition to satellite observations, the Fire Influence on Regional to Global Environments and Air Quality experiment offered sub‐orbital enhanced‐MODIS Airborne Simulator (eMAS) imagery at 50 m pixel resolution—including multiple eMAS flight tracks over individual fires in short time periods. It provided opportunity to explore smoke plume characterization at various spatial and temporal scales and quantify the limitations of space sensors for describing smoke magnitude near source as well as its temporal evolution. Here we applied modified aerosol algorithm to different imagers, relaxing its masking to estimate smoke's aerosol optical depth (AOD) as close as possible to its source. We found that GEO sensors with nominal 1 km spatial resolution can match the much finer resolution eMAS retrieved mean plume AOD, as long as the retrieval spatial resolution is finer than the width of the plumes. However, the plume's maximum AOD may be drastically underestimated by satellite products.

Gas-phase catalytic hydration of I2O5 in the polluted coastal regions: Reaction mechanisms and atmospheric implications

Marine aerosols play an important role in the global aerosol system. In polluted coastal regions, ultra-fine particles have been recognized to be related to iodine-containing species and is more serious due to the impact of atmospheric pollutants. Many previous studies have identified iodine pentoxide (I2O5, IP) to be the key species in new particles formation (NPF) in marine regions, but the role of IP in the polluted coastal atmosphere is far to be fully understood. Considering the high humidity and concentrations of pollutants in the polluted coastal regions, the gas-phase hydration of IP catalyzed by sulfuric acid (SA), nitric acid (NA), dimethylamine (DMA), and ammonia (A) have been investigated at DLPNO-CCSD(T)//ωB97X-D/aug-cc-pVTZ + aug-cc-pVTZ-PP with ECP28MDF (for iodine) level of theory. The results show that the hydration of IP involves a significant energy barrier of 22.33 kcal/mol, while the pollutants SA, NA, DMA, and A all could catalyze the hydration of IP. Especially, with SA and DMA as catalysts, the hydration reactions of IP present extremely low barriers and high rate constants. It is suggested that IP is unstable under the catalysis of SA and DMA to generate iodic acid, which is the key component in NPF in marine regions. Thus, the catalytic hydration of IP is very likely to trigger the formation of iodine-containing particles. Our research provides a clear picture of the catalytic hydration of IP as well as theoretical guidance for NPF in the polluted coastal atmosphere.

The Dark Target Algorithm for Observing the Global Aerosol System: Past, Present, and Future

The Dark Target aerosol algorithm was developed to exploit the information content available from the observations of Moderate-Resolution Imaging Spectroradiometers (MODIS), to better characterize the global aerosol system. The algorithm is based on measurements of the light scattered by aerosols toward a space-borne sensor against the backdrop of relatively dark Earth scenes, thus giving rise to the name “Dark Target”. Development required nearly a decade of research that included application of MODIS airborne simulators to provide test beds for proto-algorithms and analysis of existing data to form realistic assumptions to constrain surface reflectance and aerosol optical properties. This research in itself played a significant role in expanding our understanding of aerosol properties, even before Terra MODIS launch. Contributing to that understanding were the observations and retrievals of the growing Aerosol Robotic Network (AERONET) of sun-sky radiometers, which has walked hand-in-hand with MODIS and the development of other aerosol algorithms, providing validation of the satellite-retrieved products after launch. The MODIS Dark Target products prompted advances in Earth science and applications across subdisciplines such as climate, transport of aerosols, air quality, and data assimilation systems. Then, as the Terra and Aqua MODIS sensors aged, the challenge was to monitor the effects of calibration drifts on the aerosol products and to differentiate physical trends in the aerosol system from artefacts introduced by instrument characterization. Our intention is to continue to adapt and apply the well-vetted Dark Target algorithms to new instruments, including both polar-orbiting and geosynchronous sensors. The goal is to produce an uninterrupted time series of an aerosol climate data record that begins at the dawn of the 21st century and continues indefinitely into the future.

Validation of MODIS 3 km land aerosol optical depth from NASA's EOS Terra and Aqua missions

Abstract. In addition to the standard resolution product (10 km), the MODerate resolution Imaging Spectroradiometer (MODIS) Collection 6 (C006) data release included a higher resolution (3 km). Other than accommodations for the two different resolutions, the 10 and 3 km Dark Target (DT) algorithms are basically the same. In this study, we perform global validation of the higher-resolution aerosol optical depth (AOD) over global land by comparing against AErosol RObotic NETwork (AERONET) measurements. The MODIS–AERONET collocated data sets consist of 161 410 high-confidence AOD pairs from 2000 to 2015 for Terra MODIS and 2003 to 2015 for Aqua MODIS. We find that 62.5 and 68.4 % of AODs retrieved from Terra MODIS and Aqua MODIS, respectively, fall within previously published expected error bounds of ±(0.05 + 0.2 × AOD), with a high correlation (R= 0.87). The scatter is not random, but exhibits a mean positive bias of ∼ 0.06 for Terra and ∼ 0.03 for Aqua. These biases for the 3 km product are approximately 0.03 larger than the biases found in similar validations of the 10 km product. The validation results for the 3 km product did not have a relationship to aerosol loading (i.e., true AOD), but did exhibit dependence on quality flags, region, viewing geometry, and aerosol spatial variability. Time series of global MODIS–AERONET differences show that validation is not static, but has changed over the course of both sensors' lifetimes, with Terra MODIS showing more change over time. The likely cause of the change of validation over time is sensor degradation, but changes in the distribution of AERONET stations and differences in the global aerosol system itself could be contributing to the temporal variability of validation.

AERONET-based models of smoke-dominated aerosol near source regions and transported over oceans, and implications for satellite retrievals of aerosol optical depth

Abstract. Smoke aerosols from biomass burning are an important component of the global aerosol system. Analysis of Aerosol Robotic Network (AERONET) retrievals of aerosol microphysical/optical parameters at 10 sites reveals variety between biomass burning aerosols in different global source regions, in terms of aerosol particle size and single scatter albedo (SSA). Case studies of smoke observed at coastal/island AERONET sites also mostly lie within the range of variability at the near-source sites. Differences between sites tend to be larger than variability at an individual site, although optical properties for some sites in different regions can be quite similar. Across the sites, typical midvisible SSA ranges from ~ 0.95–0.97 (sites dominated by boreal forest or peat burning, typically with larger fine-mode particle radius and spread) to ~ 0.88–0.9 (sites most influenced by grass, shrub, or crop burning, typically smaller fine-mode particle radius and spread). The tropical forest site Alta Floresta (Brazil) is closer to this second category, although with intermediate SSA ~ 0.92. The strongest absorption is seen in southern African savannah at Mongu (Zambia), with average midvisible SSA ~ 0.85. Sites with stronger absorption also tend to have stronger spectral gradients in SSA, becoming more absorbing at longer wavelengths. Microphysical/optical models are presented in detail so as to facilitate their use in radiative transfer calculations, including extension to UV (ultraviolet) wavelengths, and lidar ratios. One intended application is to serve as candidate optical models for use in satellite aerosol optical depth (AOD) retrieval algorithms. The models presently adopted by these algorithms over ocean often have insufficient absorption (i.e. too high SSA) to represent these biomass burning aerosols. The underestimates in satellite-retrieved AOD in smoke outflow regions, which have important consequences for applications of these satellite data sets, are consistent with the level of underestimated absorption.

Interactions between biomass-burning aerosols and clouds over Southeast Asia: Current status, challenges, and perspectives

The interactions between aerosols, clouds, and precipitation remain among the largest sources of uncertainty in the Earth's energy budget. Biomass-burning aerosols are a key feature of the global aerosol system, with significant annually-repeating fires in several parts of the world, including Southeast Asia (SEA). SEA in particular provides a “natural laboratory” for these studies, as smoke travels from source regions downwind in which it is coupled to persistent stratocumulus decks. However, SEA has been under-exploited for these studies. This review summarizes previous related field campaigns in SEA, with a focus on the ongoing Seven South East Asian Studies (7-SEAS) and results from the most recent BASELInE deployment. Progress from remote sensing and modeling studies, along with the challenges faced for these studies, are also discussed. We suggest that improvements to our knowledge of these aerosol/cloud effects require the synergistic use of field measurements with remote sensing and modeling tools.

Aerosol indirect effects from shipping emissions: sensitivity studies with the global aerosol-climate model ECHAM-HAM

Abstract. In this study, we employ the global aerosol-climate model ECHAM-HAM to globally assess aerosol indirect effects (AIEs) resulting from shipping emissions of aerosols and aerosol precursor gases. We implement shipping emissions of sulphur dioxide (SO2), black carbon (BC) and particulate organic matter (POM) for the year 2000 into the model and quantify the model's sensitivity towards uncertainties associated with the emission parameterisation as well as with the shipping emissions themselves. Sensitivity experiments are designed to investigate (i) the uncertainty in the size distribution of emitted particles, (ii) the uncertainty associated with the total amount of emissions, and (iii) the impact of reducing carbonaceous emissions from ships. We use the results from one sensitivity experiment for a detailed discussion of shipping-induced changes in the global aerosol system as well as the resulting impact on cloud properties. From all sensitivity experiments, we find AIEs from shipping emissions to range from −0.32 ± 0.01 W m−2 to −0.07 ± 0.01 W m−2 (global mean value and inter-annual variability as a standard deviation). The magnitude of the AIEs depends much more on the assumed emission size distribution and subsequent aerosol microphysical interactions than on the magnitude of the emissions themselves. It is important to note that although the strongest estimate of AIEs from shipping emissions in this study is relatively large, still much larger estimates have been reported in the literature before on the basis of modelling studies. We find that omitting just carbonaceous particle emissions from ships favours new particle formation in the boundary layer. These newly formed particles contribute just about as much to the CCN budget as the carbonaceous particles would, leaving the globally averaged AIEs nearly unaltered compared to a simulation including carbonaceous particle emissions from ships.

Preface to special section on Yoram J. Kaufman Symposium on Aerosols, Clouds, and Climate

Preface to special section on Yoram J. Kaufman Symposium on Aerosols, Clouds, and Climate

Emission-Induced Nonlinearities in the Global Aerosol System: Results from the ECHAM5-HAM Aerosol-Climate Model

AbstractIn a series of simulations with the global ECHAM5-HAM aerosol-climate model, the response to changes in anthropogenic emissions is analyzed. Traditionally, additivity is assumed in the assessment of the aerosol climate impact, as the underlying bulk aerosol models are largely constrained to linearity. The microphysical aerosol module HAM establishes degrees of freedom for nonlinear responses of the aerosol system. In this study’s results, aerosol column mass burdens respond nonlinearly to changes in anthropogenic emissions, manifested in alterations of the aerosol lifetimes. Specific emission changes induce modifications of aerosol cycles with unaltered emissions, indicating a microphysical coupling of the aerosol cycles. Anthropogenic carbonaceous emissions disproportionately contribute to the accumulation mode numbers close to the source regions. In contrast, anthropogenic sulfuric emissions less than proportionally contribute to the accumulation mode numbers close to the source regions and disproportionately contribute in remote regions. The additivity of the aerosol system is analyzed by comparing the changes from a simulation with emission changes for several compounds with the sum of changes of single simulations, in each of which one of the emission changes was introduced. Close to the anthropogenic source regions, deviations from additivity are found at up to 30% and 15% for the accumulation mode number burden and aerosol optical thickness, respectively. These results challenge the traditional approach of assessing the climate impact of aerosols separately for each component and demand for integrated assessments and emission strategies.

The evolution of the global aerosol system in a transient climate simulation from 1860 to 2100

Abstract. The evolution of the global aerosol system from 1860 to 2100 is investigated through a transient atmosphere-ocean General Circulation Model climate simulation with interactively coupled atmospheric aerosol and oceanic biogeochemistry modules. The microphysical aerosol module HAM incorporates the major global aerosol cycles with prognostic treatment of their composition, size distribution, and mixing state. Based on an SRES A1B emission scenario, the global mean sulfate burden is projected to peak in 2020 while black carbon and particulate organic matter show a lagged peak around 2070. From present day to future conditions the anthropogenic aerosol burden shifts generally from the northern high-latitudes to the developing low-latitude source regions with impacts on regional climate. Atmospheric residence- and aging-times show significant alterations under varying climatic and pollution conditions. Concurrently, the aerosol mixing state changes with an increasing aerosol mass fraction residing in the internally mixed accumulation mode. The associated increase in black carbon causes a more than threefold increase of its co-single scattering albedo from 1860 to 2100. Mid-visible aerosol optical depth increases from pre-industrial times, predominantly from the aerosol fine fraction, peaks at 0.26 around the sulfate peak in 2020 and maintains a high level thereafter, due to the continuing increase in carbonaceous aerosols. The global mean anthropogenic top of the atmosphere clear-sky short-wave direct aerosol radiative perturbation intensifies to −1.1 W m−2 around 2020 and weakens after 2050 to −0.6 W m−2, owing to an increase in atmospheric absorption. The demonstrated modifications in the aerosol residence- and aging-times, the microphysical state, and radiative properties challenge simplistic approaches to estimate the aerosol radiative effects from emission projections.

The aerosol-climate model ECHAM5-HAM

Abstract. The aerosol-climate modelling system ECHAM5-HAM is introduced. It is based on a flexible microphysical approach and, as the number of externally imposed parameters is minimised, allows the application in a wide range of climate regimes. ECHAM5-HAM predicts the evolution of an ensemble of microphysically interacting internally- and externally-mixed aerosol populations as well as their size-distribution and composition. The size-distribution is represented by a superposition of log-normal modes. In the current setup, the major global aerosol compounds sulfate (SU), black carbon (BC), particulate organic matter (POM), sea salt (SS), and mineral dust (DU) are included. The simulated global annual mean aerosol burdens (lifetimes) for the year 2000 are for SU: 0.80 Tg(S) (3.9 days), for BC: 0.11 Tg (5.4 days), for POM: 0.99 Tg (5.4 days), for SS: 10.5 Tg (0.8 days), and for DU: 8.28 Tg (4.6 days). An extensive evaluation with in-situ and remote sensing measurements underscores that the model results are generally in good agreement with observations of the global aerosol system. The simulated global annual mean aerosol optical depth (AOD) is with 0.14 in excellent agreement with an estimate derived from AERONET measurements (0.14) and a composite derived from MODIS-MISR satellite retrievals (0.16). Regionally, the deviations are not negligible. However, the main patterns of AOD attributable to anthropogenic activity are reproduced.

Preface to special section on Global Aerosol System

[1] This special issue brings together papers that were presented in a workshop of experts on the global aerosol system and its impacts on climate. Aerosols originate as urban haze and rural haze, and owing to long range transport of pollutants, becomes widespread aerosol layers across the globe. [2] Atmospheric aerosols play a dual role in the climate system and the hydrologic cycle (see reviews in the work of Ramanathan et al. [2001] and Kaufman et al. [2002]). Their first role is interaction with solar and thermal radiation: by scattering sunlight and reflecting a fraction of it back to space aerosols cool the climate system; by absorbing sunlight in the atmosphere aerosols further cool the surface but warm the atmosphere, changing the temperature and humidity profiles and the conditions for cloud development. [3] Aerosol particles play a second role by affecting the hydrologic cycle: serving as cloud condensation nuclei and ice nuclei, aerosols control the cloud droplet concentration and size. Higher number concentrations of submicron pollution aerosol tend to decrease the cloud droplet size and prevent or delay development of precipitation. Supermicron sea-salt particles can reintroduce precipitation and oppose the effect of pollution aerosol. These processes may cause changes in precipitation patterns to which the human civilization adapted during the last millennium, changes in cloud cover, and possible changes in the frequency of extreme events. [4] No less important is the aerosol effect on health, air quality, and agriculture that brought policy responses in Europe and North America in the last century and is affecting policy decisions in east and southern Asia today. Therefore advancements in aerosol science, together with research on the effect of greenhouse and trace gases and increased ability to predict the impact of human activity on the regional and global aerosol, can be expected to have direct impact on energy use and economic activities in nations around the world. [5] Unraveling these aerosol effects is still difficult because of the high spatial and temporal variability of sources, complex interaction of aerosol with atmospheric trace gases and clouds, and the short lifetime of aerosol of about a week, owing to wet and dry depositions. A single aerosol particle over the Mediterranean Sea can include anthropogenic sulfate and carbonaceous material from Europe, coating natural dust particle from Africa. [6] Today’s aerosol assessments of climate are based on aerosol chemical transport models and climate models that cannot yet resolve the aerosol interaction with clouds with their microscale physical and chemical exchanges. Models make good progress in capturing aerosol evolution, but source characterization is difficult. Accurate assessments of aerosol distribution and composition, the anthropogenic component, and the impacts on radiation and water cycle therefore require orchestrated observations of aerosol, precursor trace gases, clouds and precipitation from satellites, networks of surface-based instruments, laboratory studies, and dedicated field experiments. The observations require sufficient information content, accuracy, and global coverage to permit their integration into and testing of aerosol chemical transport, assimilation, and climate models [Intergovernmental Panel on Climate Change (IPCC), 2001]. [7] In the last decade, research of the global aerosol system was invigorated by an array of new measurements in several temporal and spatial scales, the fruits of which we start to see in this special issue, and the development of new models: [8] 1. Global, daily, and multidaily observations of aerosol, clouds, and their properties derived from satellite measurements of the scattered solar light, utilizing its spectral, angular, and polarization properties. [9] 2. Satellite measurements of the vertical distribution of aerosol, clouds, and precipitation using lidars and radars and thermal infrared and microwave radiometers. [10] 3. Surface networks that continuously measure in situ and remotely (both passive radiometers and active sensors) the aerosol physical and chemical properties, distribution of solar radiation, clouds, and precipitation. [11] 4. Intensive field campaigns that concentrate the measurement power in a given region for a limited period of time and help understand the aerosol sources and aerosol and cloud processes. [12] 5. Laboratory analysis of aerosol particles and measurements of aerosol processes. [13] 6. Development of transport models that start to mimic the aerosol distribution measured from satellite and surface networks. [14] 7. Assimilation of the aerosol models and measurements into climate models to study the effects of aerosol on JOURNAL OF GEOPHYSICAL RESEARCH, VOL. 110, D10S01, doi:10.1029/2004JD005724, 2005