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Aerosol forcing uncertainty represents the largest climate forcing uncertainty overall. Its magnitude has remained virtually undiminished over the past 20 years despite considerable advances in understanding most of the key contributing elements. Recent work has produced modest increases only in the confidence of the uncertainty estimate itself. This review summarizes the contributions toward reducing the uncertainty in the aerosol forcing of climate made by satellite observations, measurements taken within the atmosphere, as well as modeling and data assimilation. We adopt a more measurement-oriented perspective than most reviews of the subject in assessing the strengths and limitations of each; gaps and possible ways to fill them are considered. Currently planned programs supporting advanced, global-scale satellite and surface-based aerosol, cloud, and precursor gas observations, climate modeling, and intensive field campaigns aimed at characterizing the underlying physical and chemical processes involved, are all essential. But in addition, new efforts are needed: (a) to obtain systematic aircraft in situ measurements capturing the multi-variate probability distribution functions of particle optical, microphysical, and chemical properties (and associated uncertainty estimates), as well as co-variability with meteorology, for the major aerosol airmass types; (b) to conceive, develop, and implement a suborbital (aircraft plus surface-based) program aimed at systematically quantifying the cloud-scale microphysics, cloud optical properties, and cloud-related vertical velocities associated with aerosol-cloud interactions; and (c) to focus much more research on integrating the unique contributions of satellite observations, suborbital measurements, and modeling, to reduce the persistent uncertainty in aerosol climate forcing.

Aerosols, the small, suspended liquid and solid particles in the atmosphere, have myriad effects on climate, weather, and air quality. When the NASA Earth-Observing System’s (EOS) Terra and Aqua satellites launched in 1999 and 2002, they each included many advanced sensors that have been used for aerosol research. In particular, the MODerate-resolution Imaging Spectroradiometer (MODIS) deployed on both satellites, has provided key data relating to aerosol loading and relative aerosol type on the global scale. Three different algorithms, known as “Dark Target”, “Deep Blue” and “MAIAC”, use different subsets of MODIS measurements and different assumptions to create various products such as Aerosol Optical Depth (AOD), fine mode fraction (FMF) and single scattering albedo (SSA). Although all three derive AOD in cloud-free conditions, each algorithm has different strengths and weaknesses in different areas of the globe and under different conditions. Here, we provide a short summary of each algorithm, description of products, and basic information about downloading and using the products. We also provide some examples of how MODIS aerosol products are used. Finally, we add a quick discussion about how these algorithms and products will continue after MODIS leaves orbit.

Although satellite retrievals and data assimilation have progressed to where there is a good skill for monitoring maritime Aerosol Optical Depth (AOD), there remains uncertainty in achieving further degrees of freedom, such as distinguishing fine and coarse mode dominated species in maritime environments (e.g., coarse mode sea salt and dust versus fine mode terrestrial anthropogenic emissions, biomass burning, and maritime secondary production). For the years 2016 through 2019, we performed an analysis of 550 nm total AOD550, fine mode AOD (FAOD550; also known as FM AOD in the literature), coarse mode AOD (CAOD550), and fine mode fraction (η550) between Moderate Resolution Spectral Imaging Radiometer (MODIS) V6.1 MOD/MYD04 dark target aerosol retrievals and the International Cooperative for Aerosol Prediction (ICAP) core four multi-model consensus (C4C) of analyses/short term forecasts that assimilate total MODIS AOD550. Differences were adjudicated by the global shipboard Maritime Aerosol Network (MAN) and selected island AERONET sun photometer observations with the application of the spectral deconvolution algorithm (SDA). Through a series of conditional and regional analyses, we found divergence included regions of terrestrial influence and latitudinal dependencies in the remote oceans. Notably, MODIS and the C4C and its members, while having good correlations overall, have a persistent +0.04 to +0.02 biases relative to MAN and AERONET for typical AOD550 values (84th% < 0.28), with the C4C underestimating significant events thereafter. Second, high biases in AOD550 are largely associated with the attribution of the fine mode in satellites and models alike. Thus, both MODIS and C4C members are systematically overestimating AOD550 and FAOD550 but perform better in characterizing the CAOD550. Third, for MODIS, findings are consistent with previous reports of a high bias in the retrieved Ångström Exponent, and we diagnosed both the optical model and cloud masking as likely causal factors for the AOD550 and FAOD550 high bias, whereas for the C4C, it is likely from secondary overproduction and perhaps numerical diffusion. Fourth, while there is no wind-speed-dependent bias for surface winds <12 m s−1, the C4C and MODIS AOD550s also overestimate CAOD550 and FAOD550, respectively, for wind speeds above 12 m/s. Finally, sampling bias inherent in MAN, as well as other circumstantial evidence, suggests biases in MODIS are likely MODIS and the C4C products have their own strengths and challenges for a given climate application and discuss needed research. even larger than what was diagnosed here. We conclude with a discussion on how

This work serves as the second of a two-part study to improve surface PM2.5 forecasts in the continental U.S. through the integrated use of multi satellite aerosol optical depth (AOD) products (MODIS Terra/Aqua and VIIRS DT/DB), multichemical transport model (CTM) (GEOS-Chem, WRF-Chem, and CMAQ) outputs, and ground observations. In Part I of the study, an ensemble Kalman filter (KF) technique using three CTM outputs and ground observations was developed to correct forecast bias and generate a single best forecast of PM2.5 for next day over non rural areas that have surface PM2.5 measurements in the proximity of 125 km. Here, with AOD data, we extended the bias correction into rural areas where the closest air quality monitoring station is at least 125–300 km away. First, we ensembled all of satellite AOD products to yield the single best AOD. Second, we corrected daily PM2.5 in rural areas from multiple models through the AOD spatial pattern between these areas and non rural areas, referred to as “extended ground truth” or EGT, for the present day. Lastly, we applied the KF technique to reduce the forecast bias for next day using the EGT. Our results find that the ensemble of bias-corrected daily PM2.5 from three CTMs for both today and next day show the best performance. Together, the two-part study develops a multimodel and multi-AOD bias-correction technique that has the potential to improve PM2.5 forecasts in both rural and non rural areas in near real time, and be readily implemented at state levels.

The widely used Moderate Resolution Imaging Spectroradiometer (MODIS) Dark-Target (DT) aerosol product fails to accurately retrieve Aerosol Optical Depth (AOD) over shallow and turbid Coastal Waters (CWs). To fill in gaps, and to improve land to ocean AOD continuity, we developed a coastal water retrieval algorithm at a spatial resolution of 1 km (CW-1km). CW-1km relies on observed top-of-atmosphere reflectance at 2.1 μm (ρ2.1), both to derive AOD and to perform a spatial variation test that enhances the existing DT masks for clouds and land. We show that the CW-1km improves spatial continuity of AOD between land, coast, and open ocean, while also increasing AOD product availability by 47.0%. Comparing with 15 years of marine aerosol network measurements, CW-1km AODs are validated to have a normalized mean bias of 1.0%, which is much smaller than 17.6% for the original DT product.

Pakistan ranks third in the world in terms of mortality attributable to air pollution, with aerosol mass concentrations (PM2.5) consistently well above WHO (World Health Organization) air quality guidelines (AQG). However, regulation is dependent on a sparse network of air quality monitoring stations and insufficient ground data. This study utilizes long-term observations of aerosols and trace gases to characterize and rank the air pollution scenarios and pollution characteristics of 80 selected cities in Pakistan. Datasets used include (1) the Aqua and Terra (AquaTerra) MODIS (Moderate Resolution Imaging Spectroradiometer) Level 2 Collection 6.1 merged Dark Target and Deep Blue (DTB) aerosol optical depth (AOD) retrieval products; (2) the CAMS (Copernicus Atmosphere Monitoring Service) reanalysis PM1, PM2.5, and PM10 data; (3) the MERRA-2 (Modern-Era Retrospective analysis for Research and Applications, Version 2) reanalysis PM2.5 data, (4) the OMI (Ozone Monitoring Instrument) tropospheric vertical column density (TVCD) of nitrogen dioxide (NO2), and VCD of sulfur dioxide (SO2) in the Planetary Boundary Layer (PBL), (5) the VIIRS (Visible Infrared Imaging Radiometer Suite) Nighttime Lights data, (6) MODIS Collection 6 Version 2 global monthly fire location data (MCD14ML), (7) population density, (8) MODIS Level 3 Collection 6 land cover types, (9) AERONET (AErosol RObotic NETwork) Version 3 Level 2.0 data, and (10) ground-based PM2.5 concentrations from air quality monitoring stations. Potential Source Contribution Function (PSCF) analyses were performed by integrating with ground-based PM2.5 concentrations and the NOAA (National Oceanic and Atmospheric Administration) HYSPLIT (Hybrid Single-Particle Lagrangian Integrated Trajectory) air parcel back trajectories to identify potential pollution source areas which are responsible for extreme air pollution in Pakistan. Results show that the ranking of the top polluted cities depends on the type of pollutant considered and the metric used. For example, Jhang, Multan, and Vehari were characterized as the top three polluted cities in Pakistan when considering AquaTerra DTB AOD products; for PM1, PM2.5, and PM10 Lahore, Gujranwala, and Okara were the top three; for tropospheric NO2 VCD Lahore, Rawalpindi, and Islamabad and for PBL SO2 VCD Lahore, Mirpur, and Gujranwala. The results demonstrate that Pakistan’s entire population has been exposed to high PM2.5 concentrations for many years, with a mean annual value of 54.7 μg/cu. m, over all Pakistan from 2003 to 2020. This value exceeds Pakistan’s National Environmental Quality Standards (Pak-NEQS, i.e., <15 μg/cu. m annual mean) for ambient air defined by the Pakistan Environmental Protection Agency (Pak-EPA) as well as the WHO Interim Target-1 (i.e., mean annual PM2.5 <35 μg/cu. m). The spatial analyses of the concentrations of aerosols and trace gases in terms of population density, nighttime lights, land cover types, and fire location data, and the PSCF analysis indicate that Pakistan’s air quality is strongly affected by anthropogenic sources inside of Pakistan, with contributions from surrounding countries. Statistically significant positive (increasing) trends in PM1, PM2.5, PM10, tropospheric NO2 VCD, and SO2 VCD were observed in ~89%, ~67%, ~48%, 91%, and ~88% of the Pakistani cities (80 cities), respectively. This comprehensive analysis of aerosol and trace gas levels, their characteristics in spatio-temporal domains, and their trends over Pakistan, is the first of its kind. Results will be helpful to the Ministry of Climate Change (Government of Pakistan), Pak-EPA, SUPARCO (Pakistan Space and Upper Atmosphere Research Commission), policymakers, and the local research community to mitigate air pollution and its effects on human health.

Satellite aerosol products such as the Dark Target (DT) produced from the MODerate resolution Imaging Spectroradiometer (MODIS) are useful for monitoring the progress of air pollution. Unfortunately, the DT often fails to retrieve during the heaviest aerosol events as well as the more moderate events in winter. Some of the literature at-tributes this lack of retrieval to the cloud mask. However, we found this lack of retrieval is mainly traced to thresholds used for masking of inland water and snow. Modifications to these two masks greatly increase 50 % of the retrievals of aerosol optical depth at 0.55 μm (AOD) greater than 1.0. The “extra”-high-AOD retrievals tend to be biased when com-pared with a ground-based sun photometer (AErosol RObotic NETwork, AERONET). Reducing bias in new retrievals re-quires two additional steps. One is an update to the assumed aerosol optical properties (aerosol model); the haze in this region is both less absorbing and lower in altitude than what is assumed in the global algorithm. The second is account-ing for the scale height of the aerosol, specifically that the heavy-aerosol events in the region are much closer to the surface than what is assumed by the global DT algorithm. The resulting combination of modified masking thresholds, new aerosol model, and lower aerosol layer scale height was applied to 3 months of MODIS observations (January–March2013) over eastern China. After these two additional steps are implemented, the significant increase in new retrievals introduces no overall bias at a high-AOD regime but does degrade other overall validation statistics. We also find that the research algorithm is able to identify additional pollution events that AERONET instruments may not due to different spatial sampling. Mean AOD retrieved from the re-search algorithm increases from 0.11 to 0.18 compared to values calculated from the operational DT algorithm during January to March of 2013 over the study area. But near Beijing, where the severe pollution occurs, the new algorithm increases AOD by as much as 3.0 for each 0.5°grid box over the previous operational-algorithm values.

Following past studies to quantify decadal trends in global carbon monoxide (CO) using satellite observations, we update estimates and find a CO trend in column amounts of about −0.50 % per year between 2002 to 2018, which is a deceleration compared to analyses performed on shorter records that found −1 % per year. Aerosols are co-emitted with CO from both fires and anthropogenic sources but with a shorter lifetime than CO. A combined trend analysis of CO and aerosol optical depth (AOD) measurements from space helps to diagnose the drivers of regional differences in the CO trend. We use the long-term records of CO from the Measurements of Pollution in the Troposphere (MOPITT) and AOD from the Moderate Resolution Imaging Spectroradiometer (MODIS) instrument. Other satellite instruments measuring CO in the thermal infrared, AIRS, TES, IASI, and CrIS, show consistent hemispheric CO variability and corroborate results from the trend analysis performed with MOPITT CO. Trends are examined by hemisphere and in regions for 2002 to 2018, with uncertainties quantified. The CO and AOD records are split into two sub-periods (2002 to 2010 and 2010 to 2018) in order to assess trend changes over the 16 years. We focus on four major population centers: Northeast China, North India, Europe, and Eastern USA, as well as fire-prone regions in both hemispheres. In general, CO declines faster in the first half of the record compared to the second half, while AOD trends show more variability across regions. We find evidence of the atmospheric impact of air quality management policies. The large decline in CO found over Northeast China is initially associated with an improvement in combustion efficiency, with subsequent additional air quality improvements from 2010 onwards. Industrial regions with minimal emission control measures such as North India become more globally relevant as the global CO trend weakens. We also examine the CO trends in monthly percentile values to understand seasonal implications and find that local changes in biomass burning are sufficiently strong to counteract the global downward trend in atmospheric CO, particularly in late summer.

To better understand and characterize current uncertainties in the important observational constraint of climate models of aerosol optical depth (AOD), we evaluate and intercompare 14 satellite products, representing nine different retrieval algorithm families using observations from five different sensors on six different platforms. The satellite products (super-observations consisting of 1°×1° daily aggregated retrievals drawn from the years 2006, 2008 and 2010) are evaluated with AErosol RObotic NETwork (AERONET) and Maritime Aerosol Network (MAN) data. Results show that different products exhibit different regionally varying biases (both under- and overestimates) that may reach ±50 %, although a typical bias would be 15 %–25 % (depending on the product). In addition to these biases, the products exhibit random errors that can be 1.6 to 3 times as large. Most products show similar performance, although there are a few exceptions with either larger biases or larger random errors. The intercomparison of satellite products extends this analysis and provides spatial context to it. In particular, we show that aggregated satellite AOD agrees much better than the spatial coverage (often driven by cloud masks) within the 1°×1° grid cells. Up to ∼50 % of the difference between satellite AOD is attributed to cloud contamination. The diversity in AOD products shows clear spatial patterns and varies from 10 % (parts of the ocean) to 100 % (central Asia and Australia). More importantly, we show that the diversity may be used as an indication of AOD uncertainty, at least for the better performing products. This provides modellers with a global map of expected AOD uncertainty in satellite products, allows assessment of products away from AERONET sites, can provide guidance for future AERONET locations and offers suggestions for product improvements. We account for statistical and sampling noise in our analyses. Sampling noise, variations due to the evaluation of different subsets of the data, causes important changes in error metrics. The consequences of this noise term for product evaluation are discussed.

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.

The state-of-art satellite observations of atmospheric aerosols over the last two decades from NASA's MODIS instruments have been extensively utilized in climate change and air quality research and applications. The operational algorithms now produce level 2 aerosol data at varying spatial resolutions (1, 3, and 10 km) and level 3 data at 1 degree. The local and global applications have been benefited from the coarse resolution gridded data sets (i.e., level 3, 1 degree), as it is easier to use since data volume is low and, several online and offline tools are readily available to access and analyze the data with minimal computing resources. At the same time, researchers who require data at much finer spatial scales have to go through a challenging process of obtaining, processing, and analyzing larger volumes of data sets that require high-end computing resources and coding skills. Therefore, we have created a high spatial resolution (HRG, 0.1x0.1 degree) daily and monthly aerosol optical depth (AOD) product by combining two MODIS operational algorithms, namely Deep Blue (DB) and Dark Target (DT). The new HRG AODs meets the accuracy requirements of level 2 AOD data and provide either the same or more spatial coverage on daily and monthly scales. The data sets are provided in daily and monthly files through open Ftp server with python scripts to read and map the data. The reduced data volume with an easy to use format and tools to access the data will encourage more users to utilize the data for research and applications.

Exposure to outdoor fine particulate matter (PM2.5) is a leading risk factor for mortality. We develop global estimates of annual PM2.5 concentrations and trends for 1998–2018 using advances in satellite observations, chemical transport modeling, and ground-based monitoring. Aerosol optical depths (AODs) from advanced satellite products including finer resolution, increased global coverage, and improved long-term stability are combined and related to surface PM2.5 concentrations using geophysical relationships between surface PM2.5 and AOD simulated by the GEOS-Chem chemical transport model with updated algorithms. The resultant annual mean geophysical PM2.5 estimates are highly consistent with globally distributed ground monitors (R2 = 0.81; slope = 0.90). Geographically weighted regression is applied to the geophysical PM2.5 estimates to predict and account for the residual bias with PM2.5 monitors, yielding even higher cross validated agreement (R2 = 0.90–0.92; slope = 0.90–0.97) with ground monitors and improved agreement compared to all earlier global estimates. The consistent long-term satellite AOD and simulation enable trend assessment over a 21 year period, identifying significant trends for eastern North America (−0.28 ± 0.03 μg/m3/yr), Europe (−0.15 ± 0.03 μg/m3/yr), India (1.13 ± 0.15 μg/m3/yr), and globally (0.04 ± 0.02 μg/m3/yr). The positive trend (2.44 ± 0.44 μg/m3/yr) for India over 2005–2013 and the negative trend (−3.37 ± 0.38 μg/m3/yr) for China over 2011–2018 are remarkable, with implications for the health of billions of people.

Emissions and long-range transport of mineral dust and combustion-related aerosol from burning fossil fuels and biomass vary from year to year, driven by the evolution of the economy and changes in meteorological conditions and environmental regulations. This study offers both satellite and model perspectives of interannual variability and possible trend of combustion aerosol and dust in major continental outflow regions over the past 15 years (2003-2017). The decade-long record of aerosol optical depth (AOD, denoted as t), separately for combustion aerosol (τ(sub c)) and dust (τ(sub d)), over global oceans is derived from the Collection 6 aerosol products of the Moderate Resolution Imaging Spectroradiometer (MODIS) onboard both Terra and Aqua. These MODIS/Aqua datasets, complemented by aerosol source-tagged simulations using the Community Atmospheric Model Version 5 (CAM5), are then analyzed to understand the interannual variability and potential trend of τ(sub c) and τ(sub d) in the major continental outflows. Both MODIS and CAM5 consistently yield a similar decreasing trend of -0.017 to - 0.020 decade(exp -1) for τ(sub c) over the North Atlantic Ocean and the Mediterranean Sea that is attributable to reduced emissions from North America and Europe, respectively. On the contrary, both MODIS and CAM5 display an increasing trend of +0.017 to +0.036 decade(exp -1) for τ(sub c) over the tropical Indian Ocean, the Bay of Bengal, and the Arabian Sea, which reflects the influence of increased anthropogenic emissions from South Asia and Middle East in the last two decades. Over the northwestern Pacific Ocean that is often affected by East Asian emissions of pollution and dust, the MODIS retrievals show a decreasing trend of - 0.021 decade(exp -1) for τ(sub c) and -0.012 decade(exp -1) for τ(sub d), which is however not reproduced by the CAM5 model. In other outflow regions strongly influenced by biomass burning smoke or dust, both MODIS retrievals and CAM5 simulations show no statistically significant trends; and the MODIS observed interannual variability is usually larger than that of the CAM5 simulation.

Given the importance of aerosol particles to radiative transfer via aerosol-radiation interactions, a methodology for tracking and diagnosing causes of temporal changes in regional-scale aerosol populations is illustrated. The aerosol optical properties tracked include estimates of total columnar burden (aerosol optical depth, AOD), dominant size mode (Ångström exponent, AE), and relative magnitude of radiation scattering versus absorption (single scattering albedo, SSA), along with metrics of the structure of the spatial field of these properties. Over well-defined regions of North America, there are generally negative temporal trends in mean and extreme AOD, and SSA. These are consistent with lower aerosol burdens and transition towards a relatively absorbing aerosol, driven primarily by declining sulfur dioxide emissions. Conversely, more remote regions are characterized by increasing mean and extreme AOD that is attributed to increased local wildfire emissions and long-range (transcontinental) transport. Regional and national reductions in anthropogenic emissions of aerosol precursors are leading to declining spatial autocorrelation in the aerosol fields and increased importance of local anthropogenic emissions in dictating aerosol burdens. However, synoptic types associated with high aerosol burdens are intensifying (becoming more warm and humid), and thus changes in synoptic meteorology may be offsetting aerosol burden reductions associated with emissions legislation.

The MEdium Resolution Imaging Spectrometer (MERIS) instrument on board ESA Envisat made measurements from 2002 to 2012. Although MERIS was limited in spectral coverage, accurate Aerosol Optical Thickness (AOT) from MERIS data are retrieved by using appropriate additional information. We introduce a new AOT retrieval algorithm for MERIS over land surfaces, referred to as eXtensible Bremen AErosol Retrieval (XBAER). XBAER is similar to the dark-target (DT) retrieval algorithm used for Moderate-resolution Imaging Spectroradiometer (MODIS), in that it uses a lookup table (LUT) to match to satellite-observed reflectance and derive the AOT. Instead of a global parameterization of surface spectral reflectance, XBAER uses a set of spectral coefficients to prescribe surface properties. In this manner, XBAER is not limited to dark surfaces (vegetation) and retrieves AOT over bright surface (desert, semiarid, and urban areas). Preliminary validation of the MERIS-derived AOT and the ground-based Aerosol Robotic Network (AERONET) measurements yield good agreement, the resulting regression equation is y (0.92 x +/- 0.07) + (0.05 +/- 0.01) and Pearson correlation coefficient of R 0.78. Global monthly means of AOT have been compared from XBAER, MODIS and other satellite-derived datasets.