Coarse Mode Aerosol Optical Depth Research Articles

Unveiling global land fine- and coarse-mode aerosol dynamics from 2005 to 2020 using enhanced satellite-based monthly inversion data

Accurate fine-mode and coarse-mode aerosol knowledge is crucial for understanding their impacts on the climate and Earth's ecosystems. However, current satellite-based Fine-Mode Aerosol Optical Depth (FAOD) and Coarse-Mode Aerosol Optical Depth (CAOD) methods have drawbacks including inaccuracies, low spatial coverage, and limited temporal duration. To overcome these issues, we developed new global-scale FAOD and CAOD from 2005 to 2020 using a novel deep learning model capable of the synergistic retrieval of two aerosol sizes. After validation with the aerosol robotic network (AERONET) and sky radiometer network (SKYNET), the new monthly FAOD and CAOD showed significant improvements in accuracy and spatial coverage. From 2005 to 2020, the new data showed that China had the greatest decrease in FAOD and CAOD. In contrast, India and South Latin America had a significant increase in FAOD versus North Africa in CAOD. FAOD in the regions of Argentina, Paraguay, and Uruguay in South America have shown an upward trend. The results reveal that FAOD and CAOD display distinct patterns of change in the same regions, particularly on the west coast of the United States where FAOD is increasing, while CAOD is decreasing. Aside from the year 2020 due to the global COVID-19 pandemic, the analysis showed that although China has seen at least an +85% increase in energy consumption and urban expansion in 2019 compared to 2005 due to the needs of development and construction, the implementation of China's air pollution control policies has led to a significant decrease in FAOD (−46%) and CAOD (−65%) after 2013. This research enriches our comprehension of global fine and coarse aerosol patterns, additional investigations are needed to determine the potential global implications of these changes.

Estimation of pan-European, daily total, fine-mode and coarse-mode Aerosol Optical Depth at 0.1° resolution to facilitate air quality assessments

Aerosol Optical Depth (AOD) data derived from satellites is crucial for estimating spatially-resolved PM concentrations, but existing AOD data over land remain affected by several limitations (e.g., data gaps, coarser resolution, higher uncertainty or lack of size fraction data), which weakens the AOD-PM relationship. We developed a 0.1° resolution daily AOD data set over Europe over the period 2003–2020, based on two-stage Quantile Machine Learning (QML) frameworks. Our approach first fills gaps in satellite AOD data and then constructs three components' models to obtain reliable full-coverage AOD along with Fine-mode AOD (fAOD) and Coarse-mode AOD (cAOD). These models are based on AERONET (AErosol RObotic NETwork) observations, Gap-filled satellite AOD, climate and atmospheric composition reanalyses. Our QML AOD products exhibit better quality with an out-of-sample R2 equal to 0.68 for AOD, 0.66 for fAOD and 0.65 for cAOD, which is 23–92 %, 11–13 % and 115–132 % higher than the corresponding satellite or reanalysis products, respectively. Over 91.6 %, 81.6 %, and 88.9 % of QML AOD, fAOD and cAOD predictions fall within ±20 % Expected Error (EE) envelopes, respectively. Previous studies reported that a weak satellite AOD-PM correlation across Europe (Pearson correlation coefficient (PCC) around 0.1). Our QML products exhibit higher correlations with ground-level PMs, particularly when broadly matched by size: AOD with PM10, fAOD with PM2.5, cAOD with PM coarse (R = 0.41, 0.45 and 0.26, respectively). Different AOD fractions more effectively distinct PM size fractions, than total AOD. Our QML aerosol dataset and models pioneer full-coverage, daily high-resolution monitoring of fine-mode and coarse-mode aerosols, effectively addressing existing AOD challenges for further PMs exposures' estimations. This dataset opens avenues for more in-depth exploration of the impacts of aerosols on human health, climate, visibility, and biogeochemical processes, offering valuable insights for air quality management and environmental health risk assessment.

Detection and analysis of Lhù'ààn Mân' (Kluane Lake) dust plumes using passive and active ground-based remote sensing supported by physical surface measurements

Abstract. There is growing recognition that high-latitude dust (HLD), originating from local drainage-basin flows, is the dominant source for certain important phenomena such as particle deposition on snow/ice. The analysis of such local plumes (including a better exploitation of remote sensing data) has been targeted as a key aerosol issue by the HLD community. The sub-Arctic Lhù'ààn Mân' (Kluane Lake) region in the Canadian Yukon is subject to regular drainage-basin, wind-induced dust plumes. This dust emission site is one of many current and potential proglacial dust sources in the Canadian north. In situ ground-based measurements are, due to constraints in accessing these types of regions, rare. Ground- and satellite-based remote sensing accordingly play an important role in helping to characterize local dust sources in the Arctic and sub-Arctic. We compared ground-based passive and active remote sensing springtime (May 2019) retrievals with microphysical surface-based measurements in the Lhù'ààn Mân' region in order to better understand the potential for ground- and satellite-based remote sensing of HLD plumes. This included correlation analyses between ground-based coarse mode (CM) aerosol optical depth (AOD) retrievals from AERONET AOD spectra, CM AODs derived from co-located Doppler lidar profiles, and OPS (optical particle sizer) surface measurements of CM particle-volume concentration (vc(0)). An automated dust classification scheme was developed to objectively identify local dust events. The classification process helped distinguish lidar-derived CM AODs which covaried with vdust(0) (during recognized dust events) and those that varied at the same columnar scale as AERONET-derived CM AOD (and thus could be remotely sensed). False positive cloud events for dust-induced, high-frequency variations in lidar-derived CM AODs in cloudless atmospheres indicated that the AERONET cloud-screening process was rejecting CM dust AODs. The persistence of a positive lidar ratio bias in comparing the CIMEL/lidar-derived value with a prescribed value obtained from OPS-derived particle sizes coupled with dust-speciation-derived refractive indices led to the suggestion that the prescribed value could be increased to optically derived values of 20 sr by the presence of optically significant dust particles at an effective radius of 11–12 µm. Bimodal CM PSDs (see Appendix B for a glossary) from full-fledged AERONET inversions (the combination of AOD spectra and almucantar radiances) also showed CM peaks at ∼ 1.3 and 5–6.6 µm radius: this, we argue, was associated with springtime Asian dust and Lhù'ààn Mân' dust, respectively. Correlations between the CIMEL-derived fine mode (FM) AOD and FM OPS-derived particle-volume concentrations suggest that remote sensing techniques can be employed to monitor FM dust (which is arguably a better indicator of the long-distance transport of HLD).

Understanding day–night differences in dust aerosols over the dust belt of North Africa, the Middle East, and Asia

Abstract. Utilizing the well-calibrated, high-spectral-resolution equal-quality performance of daytime and nighttime (09:30 and 21:30 local solar Equator-crossing time (local solar ECT)) products of the Infrared Atmospheric Sounder Interferometer (IASI) from the Laboratoire de Météorologie Dynamique (LMD), this study investigates the day–night differences in dust aerosols over the global dust belt of North Africa, the Middle East, and Asia. Both daytime dust optical depth (DOD) and nighttime DOD at 10 µm show high consistency with solar and lunar observations of coarse-mode aerosol optical depth (CAOD) from AErosol RObotic NETwork (AERONET) sites across the dust belt, with correlation coefficients of 0.8–0.9 for most sites. Both IASI DOD and dust layer height show a significant (95 % confidence level) day–night difference over the major dust sources within the dust belt. Daytime DOD over the central to northern Sahara, the central to eastern Arabian Peninsula, and the Taklamakan Desert is significantly higher than that of nighttime but lower than nighttime over the southern Sahel to the Guinea Coast and the western to central Indian subcontinent in the annual mean. The magnitude of the day–night differences in DOD is larger and more evident in boreal winter and spring than in other seasons. The positive day–night differences in DOD (i.e., higher daytime values than nighttime) over the central Sahara, the Middle East, and Asia are likely associated with greater dust emissions driven by higher dust uplift potential (DUP) and stronger wind speeds during daytime. Dust layer heights demonstrate negative day–night differences over dust source regions in the central Sahara, central Arabian Peninsula, and Taklamakan Desert and positive height differences in the southern Sahel to the Guinea Coast, southern parts of the Arabian Peninsula, and large parts of the Indian subcontinent. The higher dust layer height over the Guinea Coast and the Indian subcontinent during the daytime is associated with a deeper planetary boundary layer height and greater convective instability during daytime than nighttime, which promotes vertical transport and mixing of dust aerosols. The corresponding lower daytime DOD over the Sahel and the Indian subcontinent indicates a possible dilution of dust aerosols when they are transported to higher altitudes by convection where they are more susceptible to horizontal transport. Ground-based observations of dust show surface PM10 concentration and CAOD exhibit a spatially varying diurnal cycle across the dust belt. CAOD and PM10 concentrations generally peak in late morning and from late afternoon to midnight in the Sahel and in early afternoon and around early morning in the Middle East, the timings of which are largely consistent with the day–night differences in IASI DOD. It is also found that DOD from reanalysis products (e.g., Modern-Era Retrospective Analysis for Research and Applications, version 2 (MERRA-2) and ECMWF Atmospheric Composition Reanalysis 4 (EAC4)) failed to capture the day–night differences in IASI DOD in large parts of the dust belt except in small dust source hotspots over North Africa.

The Role of Midlatitude Cyclones in the Emission, Transport, Production, and Removal of Aerosols in the Northern Hemisphere

AbstractWe examine the distribution of aerosol optical depth (AOD) across 27,707 northern hemisphere (NH) midlatitude cyclones for 2005–2018 using retrievals from the Moderate Resolution Spectroradiometer (MODIS) sensor on the Aqua satellite. Cyclone‐centered composites show AOD enhancements of 20%–45% relative to background conditions in the warm conveyor belt (WCB) airstream. Fine mode AOD accounts for 68% of this enhancement annually. Relative to background conditions, coarse mode AOD is enhanced by more than a factor of two near the center of the composite cyclone, co‐located with high surface wind speeds. Within the WCB, MODIS AOD maximizes in spring, with a secondary maximum in summer. Cyclone‐centered composites of AOD from the Modern Era Retrospective analysis for Research and Applications, version 2 Global Modeling Initiative (M2GMI) simulation reproduce the magnitude and seasonality of the MODIS AOD composites and enhancements. M2GMI simulations show that the AOD enhancement in the WCB is dominated by sulfate (37%) and organic aerosol (25%), with dust and sea salt each accounting for 15%. MODIS and M2GMI AOD are 60% larger in North Pacific WCBs compared to North Atlantic WCBs and show a strong relationship with anthropogenic pollution. We infer that NH midlatitude cyclones account for 355 Tg yr−1 of sea salt aerosol emissions annually, or 60% of the 30–80°N total. We find that deposition within WCBs is responsible for up to 35% of the total aerosol deposition over the NH ocean basins. Furthermore, the cloudy environment of WCBs leads to efficient secondary sulfate production.

Estimating the Wind Dependency of Aerosol Optical Depth at Remote Oceanic Regions

In this article, the applicability of India’s indigenously developed scatterometer, Scatsat-1 for marine aerosol characterization and wind dependency of aerosol optical depth (AOD) was investigated using 3 years of satellite data. Wind data from Scatsat-1 and AOD with its size fraction from SNPP VIIRS from 2017 to 2019 were used for the investigation. A technique has been demonstrated for identifying remote oceanic regions with mostly marine aerosol using certain criteria like distance from land, higher fraction of coarse AOD, lower variation of AOD with wind direction, and so forth. Daily wind and AOD from 2017 to 2019 were used for studying the relationship between wind speed and AOD at remote oceanic locations away from terrestrial and anthropogenic influence. Five regions of interest (ROIs) of 5° by 5° were identified in different oceanic regions for carrying out the regression analysis. A linear increase of coarse mode AOD and total AOD with an increase in wind speed was observed for all five remote locations while fine mode AOD was unrelated. The slope of the linear relation agreed with Kiliyanpilakkil and Meskhidze (2011) for intermediate wind values. The remote regions also had a lower variation of AOD with change in wind direction implying less transport of aerosol from nearby landmasses.

Global validation and comparison of MODIS DT and POLDER-3 GRASP aerosol products over ocean

The Moderate Resolution Imaging Spectroradiometer (MODIS) and the third generation of Polarization and Directionality of Earth's Reflectances (POLDER-3) are two types of sensors, which have their own advantages in sensor design. MODIS is a conventional multi-spectral imager with single-angle observations and a wide spectral range of surface reflection bands from blue to shortwave infrared, while POLDER-3 is a multi-angle polarization instrument with narrower spectral range from blue to shortwave near-infrared. It is highly anticipated to understand the quantitative capability of these two sensors in aerosol retrievals. For this purpose, this study conducts a long-time series comparison and evaluation of over-ocean aerosol products from these two types of sensors during the period 2005–2013, corresponding to the entire lifetime of the POLDER-3 products. The MODIS aerosol products based on Dark Target (DT) algorithm and two POLDER-3 products based on General Retrieval of Atmosphere and Surface Properties (GRASP) “High Precision” (GRASP/HP) and “Models” (GRASP/Models) algorithm are adopted in this study. Two types of ground-based measurements from automatic Aerosol Robotic Network (AERONET) data and shipborne Maritime Aerosol Network (MAN) data are employed to validate four parameters common to both satellite products, including total Aerosol Optical Depth (AOD), Ångström Exponent (AE), fine-mode AOD (AODF) and coarse-mode AOD (AODC). The overall validation results show GRASP/Models has similar performance with MODIS DT in total AOD products. This indicates that the multi-angle polarization observations of POLDER-3 can have the same advantages as the multi-spectral observations of MODIS in total AOD retrievals. Furthermore, the statistical parameters of the validation results based on AERONET data show that GRASP/Models is slightly better than MODIS DT. However, for the validation results using MAN data, it is interesting to find that MODIS DT is slightly better than GRASP/Models in all aspects. This may be due that the manual measurements of MAN can consciously avoid more cloud contamination. Meanwhile, it suggests that MODIS DT algorithm over ocean needs further improvements in cloud mask and quality control. In addition, from the validation results of both types of ground-based data, it shows that GRASP/HP significantly overestimates AOD, but has better validation accuracy than GRASP/Models and MODIS DT in AE products, which implies that multi-angle polarization sensor has great potential in aerosol properties retrieval. For AODF and AODC, the statistical parameters of validation results for all three products show little difference. GRASP/HP is slightly better than GRASP/Models and MODIS DT in AODF products, while the AODC products of GRASP/Models and MODIS DT show slightly superior to that of GRASP/HP. This may suggest that although the higher AE validation accuracy of GRASP/HP, the higher total AOD accuracy of GRASP/Models and MODIS DT still dominates the validation results of AODF and AODC. The results could contribute to the application of over-ocean aerosol products of these two satellite in climate research, as well as to the improvement of aerosol retrieval algorithms over ocean for instruments such as single viewing spectrometer and multi-angle polarimeter.

Climatology of aerosol component concentrations derived from multi-angular polarimetric POLDER-3 observations using GRASP algorithm

Abstract. The study presents a climatology of aerosol composition concentrations obtained by a recently developed algorithm approach, namely the Generalized Retrieval of Atmosphere and Surface Properties (GRASP)/Component. It is applied to the whole archive of observations from the POLarization and Directionality of the Earth's Reflectances (POLDER-3). The conceptual specifics of the GRASP/Component approach is in the direct retrieval of aerosol speciation (component fraction) without intermediate retrievals of aerosol optical characteristics. Although a global validation of the derived aerosol component product is challenging, the results obtained are in line with general knowledge about aerosol types in different regions. In addition, we compare the GRASP-derived black carbon (BC) and dust components with those of the Modern-Era Retrospective Analysis for Research and Applications, version 2 (MERRA-2) product. Quite a reasonable general agreement was found between the spatial and temporal distribution of the species provided by GRASP and MERRA-2. The differences, however, appeared in regions known for strong biomass burning and dust emissions; the reasons for the discrepancies are discussed. The other derived components, such as concentrations of absorbing (BC, brown carbon (BrC), iron-oxide content in mineral dust) and scattering (ammonium sulfate and nitrate, organic carbon, non-absorbing dust) aerosols, represent scarce but imperative information for validation and potential adjustment of chemical transport models. The aerosol optical properties (e.g., aerosol optical depth (AOD), Ångström exponent (AE), single-scattering albedo (SSA), fine- and coarse-mode aerosol optical depth (AODF AND AODC)) derived from GRASP/Component were found to agree well with the Aerosol Robotic Network (AERONET) ground reference data, and were fully consistent with the previous GRASP Optimized, High Precision (HP) and Models retrieval versions applied to POLDER-3 data. Thus, the presented extensive climatology product provides an opportunity for understanding variabilities and trends in global and regional distributions of aerosol species. The climatology of the aerosol components obtained in addition to the aerosol optical properties provides additional valuable, qualitatively new insight about aerosol distributions and, therefore, demonstrates advantages of multi-angular polarimetric (MAP) satellite observations as the next frontier for aerosol inversion from advanced satellite observations. The extensive satellite-based aerosol component dataset is expected to be useful for improving global aerosol emissions and component-resolved radiative forcing estimations. The GRASP/Component products are publicly available (https://www.grasp-open.com/products/, last access: 15 March 2022) and the dataset used in the current study is registered under https://doi.org/10.5281/zenodo.6395384 (Li et al., 2022b).

A Coupled Evaluation of Operational MODIS and Model Aerosol Products for Maritime Environments Using Sun Photometry: Evaluation of the Fine and Coarse Mode

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 even larger than what was diagnosed here. We conclude with a discussion on how MODIS and the C4C products have their own strengths and challenges for a given climate application and discuss needed research.

Extensive characterization of aerosol optical properties and chemical component concentrations: Application of the GRASP/Component approach to long-term AERONET measurements

A recently developed GRASP/Component approach (GRASP: Generalized Retrieval of Atmosphere and Surface Properties) was applied to AERONET (Aeronet Robotic Network) sun photometer measurements in this study. Unlike traditional aerosol component retrieval, this approach allows the inference of some information about aerosol composition directly from measured radiance, rather than indirectly through the inversion of optical parameters, and has been integrated into the GRASP algorithm. The newly developed GRASP/Component approach was applied to 13 AERONET sites for different aerosol types under the assumption of aerosol internal mixing rules to analyze the characteristics of aerosol components and their distribution patterns. The results indicate that the retrievals can characterize well the spatial and temporal variability of the component concentration for different aerosol types. A reasonable agreement between GRASP BC retrievals and MERRA-2 BC products is found for all different aerosol types. In addition, the relationships between aerosol component content and aerosol optical parameters such as aerosol optical depth (AOD), fine-mode fraction (FMF), absorption Ångström exponent (AAE), scattering Ångström exponent (SAE), and single scattering albedo (SSA) are also analyzed for indirect verifying the reliability of the component retrieval. It was demonstrated the GRASP/Component optical retrievals are in good agreement with AERONET standard products [e.g., correlation coefficient (R) of 0.93–1.0 for AOD, fine-mode AOD (AODF), coarse-mode AOD (AODC) and Ångström exponent (AE); R = ~ 0.8 for absorption AOD (AAOD) and SSA; RMSE (root mean square error) < 0.03 for AOD, AODF, AODC, AAOD and SSA]. Thus, it is demonstrated the GRASP/Component approach can provide aerosol optical products with comparable accuracy as the AERONET standard products from the ground-based sun photometer measurements as well as some additional important inside on aerosol composition.

A global-scale analysis of the MISR Level-3 aerosol optical depth (AOD) product: Comparison with multi-platform AOD data sources

This study analyses the applicability of the recently released Level-3 (L3) daily and monthly aerosol optical depth (AOD) products (version F15_0032) over land retrieved from the Multiangle Imaging Spectroradiometer (MISR) instrument. For this purpose, daily AOD data from 427 Aerosol Robotic Network (AERONET) sites worldwide during 2001–2018 and 39 China Aerosol Remote Sensing Network (CARSNET) sites across China during 2002–2014 were selected for comparison. Also, MISR-based size-segregated AODs were collected to compare with the coarse- and fine-mode AODs retrieved from AERONET to reveal the particles size modes that mainly contribute to the offset of MISR total AOD relative to observations. By comparing with five other monthly AOD datasets, including two MODIS (Moderate resolution Imaging Spectroradiometer) retrieval products, a multi-satellite merged product, and two aerosol reanalysis, MERRA-2 (Modern-Era Retrospective Analysis for Research and Applications) and CAMS (Copernicus Atmosphere Monitoring Service), we then explored the applicability of MISR for characterizing the climatology, interannual variations, and long-term (2003–2017) trends in regional aerosol loadings over the 12 regions of interest. Overall, about 80% (60%) of the daily AOD values retrieved by MISR fall within expected error bounds of ± [0.05 + 0.2 × AOD] (±[0.03 + 0.1 × AOD]), with a high correlation (R = 0.87). Our comparison results show that although the V23 algorithm addresses several issues in L2 AOD retrieval relative to the previous version, the L3 data aggregated from L2 data tends to on average overestimate low AOD values and underestimate high AOD values. These offset relative to observations are mainly attributed to the overestimation of coarse-mode AOD and the underestimation of fine-mode AOD by MISR. Intercomparison of 2003–2017 AOD trends from multiple data sources indicate that MISR can capture well the increases occurring in South Asia, as well as the decreases occurring in Eastern China, Eastern United States, and Western Europe. Our study confirmed that MISR L3 product performs reliably at regional scales, particularly in typically polluted areas, but caution is still needed when applied to areas where sparse sampling is encountered.

Aerosol optical properties derived from POLDER-3/PARASOL (2005–2013) over the Western Mediterranean Sea – Part 2: Spatial distribution and temporal variability

Abstract. The Mediterranean atmosphere is impacted by a variety of natural and anthropogenic aerosols which exert a complex and variable pressure on the regional climate and air quality. This study focuses on the Western Mediterranean Sea (west of longitude 20∘ E) using the full POLarization and Directionality of the Earth's Reflectances version 3 (POLDER-3)/Polarization &amp;amp; Anisotropy of Reflectances for Atmospheric Sciences coupled with Observations from a Lidar (PARASOL) aerosol data record derived from the operational clear-sky ocean algorithm (collection 3) available from March 2005 to October 2013. This 8.5-year satellite data set includes retrievals at 865 nm of the total, fine-, and coarse-mode aerosol optical depth (AOD, AODF, and AODC, respectively), Ångström exponent (AE), and the spherical/non-spherical partition of the coarse-mode AOD (AODCS and AODCNS, respectively), that have been carefully validated over the study region (Formenti et al., 2018). Here, we analyze the spatial distribution, the seasonal cycle, and interannual variability of this ensemble of advanced aerosol products in three latitude bands (34–38, 38–42, and &gt; 42∘ N) and for three sites (Ersa, Barcelona, Lampedusa) distributed on the western basin. POLDER-3 retrieves the high influence of north African desert dust over the region, which largely controls the spatial distributions (south-to-north decreasing gradient) and seasonal cycles (spring/summer maximum) of both AOD and coarse AOD, including its non-spherical component. In contrast, the coarse spherical component of AOD remains relatively homogenously low all year long over the region, whereas fine-mode AODs are generally more elevated in the eastern part of the region of study, especially north of the Adriatic Sea. From 2005 to 2013, annual POLDER-3 AOD evolution shows a decreasing trend of 0.0030 yr−1 in absolute value at 865 nm (0.0060 yr−1 at 550 nm). Such a downward evolution is much more pronounced and spatially extended for AODF (−0.0020 yr−1 at 865 nm) than for AODC. Our analysis also suggests that the North Atlantic Oscillation (NAO) index explains a significant part of the interannual variability of POLDER-3 AODC, reflecting its role on the frequency of Saharan dust transport over the region. Finally, the POLDER-3 data set highlights an improvement of air quality related to the fine aerosol component, with a marked evolution toward more frequent occurrence of clean conditions (≥ 75 % of daily AODF-865 nm&lt;0.05) at the end of the period of study (2010–2013) over most of the Western Mediterranean Sea, and much less evidence of such a large-scale evolution for the coarse fraction. Therefore, despite the high and variable influence of mostly natural north African dust over the region, the POLDER-3 advanced aerosol data set appears sufficiently accurate to successfully resolve the concurrent downward trend of fine, primarily anthropogenic particles, most likely related to reduced emissions in the surrounding European countries.

Validation of the aerosol optical property products derived by the GRASP/Component approach from multi-angular polarimetric observations

The multi-angle polarimetric satellite observations are helpful for improving the retrievals of aerosol parameters. However, practical applications of polarization technology are still limited because of complexity of measurement and interpretation of polarimetric observations. In this study, we analyze the performance of a new component approach developed in the frame of the Generalized Retrieval of Atmosphere and Surface Properties (GRASP) algorithm. In addition to aerosol optical properties including particle size distribution, non-sphericity and index of refraction that are commonly derived from multi-angle radiance and polarization measurements, the GRASP/Component approach also provides some information about aerosol composition. Specifically, in this approach aerosol is modeled as an internal mixture of several components with distinctly different chemical compositions and known refractive indices. The approach is intended not only to provide additional insight on aerosol composition but also to improve retrieval of basic aerosol optical properties. This study presents comprehensive validation and evaluation of Aerosol Optical Depth (AOD), Ångström exponent (AE), fine mode AOD (AODF), coarse mode AOD (AODC), and single scattering albedo (SSA) as retrieved by the GRASP/Component approach. The GRASP/Component products include aerosol retrievals using two different aerosol component mixing rules, i.e., Maxwell-Garnett (MG) effective medium approximation and a simple Volume-Weighted averaging (VW). The differences between the results obtained using these two assumptions are also discussed. The obtained results show that the aerosol optical property products of GRASP/Component approach have good agreement with the ground-based AERONET measurements, which is comparable to other PARASOL/GRASP approaches. Specifically, the AOD retrieved by GRASP/Component approach show high correlation and nearly no bias both over land and ocean, as compared with AERONET. The more detailed aerosol properties such as AE, AODF, AODC and SSA also show one of the best comparisons with AERONET. These improvements can probably be attributed to the use of the additional physical constraints on spectral dependence of the complex refractive index and the reduction of total number of aerosol parameters directly retrieved in the GRASP/Component approach. In addition, the choice of mixing rules had no significant effect on optical retrievals. With the exception of SSA, the results obtained based on the MG mixing rule were found to be slightly better over those obtained using VW mixing rule, especially for bias.

Temporal and spatial variations of aerosol optical properties over the Korean peninsula during KORUS-AQ

We investigated the temporal and spatial variations of aerosol optical properties over the Korean peninsula during the KORUS-AQ (KORea–United States Air Quality) experiment with ground-based aerosol optical properties measured by remote and in-situ techniques. On the ground, AErosol RObotic NETwork (AERONET) and ground-level particulate matter (PM) concentration from air quality monitoring stations were used. From the NASA DC-8 research aircraft, the airborne Spectrometer for Sky-Scanning, Sun-Tracking Atmospheric Research instrument (4STAR), an aerosol mass spectrometer (AMS), and a single particle soot photometer (SP2) provided aerosol information. Average hourly fine- and coarse-mode aerosol optical depth (AOD) and fine mode fraction (FMF), were divided into four clusters (background, Seoul Metropolitan Area (SMA), southwest, and east) representing different temporal/spatial variations; the results of those clusters were similar to the clustering results using PM from air quality monitoring stations. The downwind region of SMA was dominant by light-scattering fine-mode aerosols likely due to secondary aerosol formation with high fine-mode AOD and single scattering albedo compared to other regions, even Seoul. The fine-mode aerosols were more spatially homogeneous than coarse-mode aerosols, especially in the west-to-east direction, because fine-mode aerosols are usually transported on a regional scale by westerlies rather than emitted from local emission sources. However, the aerosol size distribution was spatially more homogeneous because of a consistent contribution of fine- and coarse-mode AOD to total AOD regardless of direction between the AERONET sites. During high-aerosol loading episodes, the temporal and spatial variations of aerosol optical properties were similar to those derived from 4STAR and ground-level PM concentrations, providing detailed information on aerosol behavior and characteristics. Using missed-approach flight segments (touchdown and take-off without a full-stop), investigation of diurnal variations over the SMA revealed a significant increase in AOD and Angstrom exponent (AE) in the afternoon compared to morning and noon, especially in the downwind region, because of more active secondary formation resulting from advected and/or emitted local pollutants and precursors. The diurnal variation of PM1 in the downwind region was similar to that of AOD; it was mainly increased during the day by secondary organic aerosols and ammonium nitrate due to large amounts of isoprene and meteorological conditions that supported secondary aerosol formation. Ammonium sulfate also partially led to increasing the PM1, but its behavior was unclear, because RH decreased during the day, which would imply the reduced aqueous-phase oxidation (the major pathway for sulfate production). Compared to the downwind region, ammonium nitrate and refractory black carbon decreased in Seoul because of a slightly decreased traffic volume, dissociation of ammonium nitrate, and increased boundary layer height according to meteorological conditions in the afternoon. The results of this study provide detailed information on aerosol behavior given the synergy of the various measurement platforms used. Along with the evidence of active photochemical reactions taking place in the downwind region, such data will be useful in formulating policies that improve air quality in Korea.

Evaluation of climate model aerosol trends with ground-based observations over the last 2 decades – an AeroCom and CMIP6 analysis

Abstract. This study presents a multiparameter analysis of aerosol trends over the last 2 decades at regional and global scales. Regional time series have been computed for a set of nine optical, chemical-composition and mass aerosol properties by using the observations from several ground-based networks. From these regional time series the aerosol trends have been derived for the different regions of the world. Most of the properties related to aerosol loading exhibit negative trends, both at the surface and in the total atmospheric column. Significant decreases in aerosol optical depth (AOD) are found in Europe, North America, South America, North Africa and Asia, ranging from −1.2 % yr−1 to −3.1 % yr−1. An error and representativity analysis of the spatially and temporally limited observational data has been performed using model data subsets in order to investigate how much the observed trends represent the actual trends happening in the regions over the full study period from 2000 to 2014. This analysis reveals that significant uncertainty is associated with some of the regional trends due to time and space sampling deficiencies. The set of observed regional trends has then been used for the evaluation of 10 models (6 AeroCom phase III models and 4 CMIP6 models) and the CAMS reanalysis dataset and of their skills in reproducing the aerosol trends. Model performance is found to vary depending on the parameters and the regions of the world. The models tend to capture trends in AOD, the column Ångström exponent, sulfate and particulate matter well (except in North Africa), but they show larger discrepancies for coarse-mode AOD. The rather good agreement of the trends, across different aerosol parameters between models and observations, when co-locating them in time and space, implies that global model trends, including those in poorly monitored regions, are likely correct. The models can help to provide a global picture of the aerosol trends by filling the gaps in regions not covered by observations. The calculation of aerosol trends at a global scale reveals a different picture from that depicted by solely relying on ground-based observations. Using a model with complete diagnostics (NorESM2), we find a global increase in AOD of about 0.2 % yr−1 between 2000 and 2014, primarily caused by an increase in the loads of organic aerosols, sulfate and black carbon.

Climatological aspects of size-resolved column aerosol optical properties over a rural site in the southern peninsular India

We present the long-term (2008–2018) climatological characteristics of column aerosol optical properties from the Sky Radiometer at Gadanki (13.48∘ N, 79.18∘ E), a typical rural site in southern peninsular India. A method to separate the fine and coarse mode spectral aerosol optical properties was presented. The climatological aspects related to the diurnal, monthly, and intra-annual variations of observed aerosol optical properties exhibited both seasonal and spectral dependence. While the size-resolved aerosol optical depth (AOD), absorption aerosol optical depth, and asymmetry parameter exhibited a decreasing trend, single scattering albedo (SSA) showed an increasing trend from shorter to longer wavelengths in all seasons with distinct magnitudes. Seasonal asymmetry in the diurnal variation of AOD and Angstrom exponent was observed. Intra-annual variability clearly indicated distinct fine and coarse mode dominance during winter and monsoon, respectively, while mixed contributions were found in other seasons. This is attributed to the influence of prevailing air masses on the column aerosol properties. Annual mean SSA values indicated the dominance of moderately absorbing (0.91) to weakly absorbing (0.95) aerosols. On evaluating the size-resolved AOD (at 500 nm) with those from extended Spectral Deconvolution Algorithm (SDA+), the observed differences are found to be remarkable for coarse mode AOD although the correlations for both fine and coarse AODs were observed to be 0.96. Lastly, the Dark Target and Deep Blue merged AOD (at 550 nm) from MODIS Terra/Aqua are evaluated to examine the consistency with ground measurements and both have shown a systematic underestimation with an increase in the magnitude of AOD strongly dependent on the seasons. These results form a basis for the comprehensive characterization of aerosol types and associated radiative impacts that are vital for understanding the regional climate change.

Climatological‐Scale Analysis of Intensive and Semi‐intensive Aerosol Parameters Derived From AERONET Retrievals Over the Arctic

AbstractWe investigated the climatological‐scale, monthly binned, seasonal variation of AERONET/Dubovik retrievals across six stations in the North American and European Arctic (multiyear sampling periods ranging from 8 to 17 years). A robust, spring‐to‐summer (StoS) increase in the radius of the peak of the fine mode (FM) component of the particle size distribution (PSD) was observed for five of the six stations. The FM aerosol optical depth (AOD) and the FM effective radius at the individual stations showed, respectively, a negligible to moderate StoS decrease and a significant increase. This was interpreted as a trade‐off between the waning influence of smaller FM Arctic haze aerosols and the increasing influence of large FM smoke particles. A springtime, pan‐Arctic PSD peak in the 1.3 μm coarse mode (CM) bin was attributed to Asian dust. It was suggested that the increase in amplitude of a second (4–7 μm) CM peak from July to August at the low‐elevation coastal sites was influenced by wind‐induced sea salt. The CM AOD went through a StoS decrease attributed to the decreasing amplitude of the 1.3 μm peak. A significant StoS CM effective radius increase was ascribed to the decreasing influence of the 1.3 μm peak. StoS FM fraction increases were largely due to the decrease of the CM AOD (decreasing influence of springtime Asian dust). This extensive and intensive climatology of remotely sensed, bimodal properties will, we believe, provide an important reference for future measurements and modeling of Arctic aerosols.

Analysis of the Transport of Aerosols over the North Tropical Atlantic Ocean Using Time Series of POLDER/PARASOL Satellite Data

The time series of total, fine and coarse POLAC/PARASOL aerosol optical depth (AOD) satellite products (2005–2013) processed by the POLAC algorithm are examined to investigate the transport of aerosols over the North Tropical Atlantic Ocean, a region that is characterized by significant dust aerosols events. First, the comparison of satellite observations with ground-based measurements acquired by AERONET ground-based measurements shows a satisfactory consistency for both total AOD and coarse mode AOD (i.e., correlation coefficients of 0.75 and bias ranging from −0.03 to 0.03), thus confirming the robustness and performance of POLAC/PARASOL data to investigate the spatio-temporal variability of the aerosols over the study area. Regarding fine mode aerosol, POLAC/PARASOL data present a lower performance with correlation coefficient ranging from 0.37 to 0.73. Second, the analysis of POLAC/PARASOL aerosol climatology reveals a high contribution of the coarse mode of aerosols ( AOD c between 0.1 and 0.4) at long distance from the African sources, confirming previous studies related to dust transport. The POLAC/PARASOL data were also compared with aerosol data obtained over the North Tropical Atlantic Ocean from MACC and MERRA-2 reanalyses. It is observed that the total AOD is underestimated in both reanalysis with a negative bias reaching −0.2. In summary, our results thus suggest that satellite POLAC/PARASOL observations of fine and coarse modes of aerosols could provide additional constraints useful to improve the quantification of the dust direct radiative forcing on a regional scale but also the biogeochemical processes such as nutrient supply to the surface waters.

Sub-Mode Aerosol Volume Size Distribution and Complex Refractive Index from the Three-Year Ground-Based Measurements in Chengdu China

Chengdu is a typical basin city of Southwest China with rare observations of remote sensing measurements. To assess the climate change and establish a region aerosol model, a deeper understanding of the separated volume size distribution (VSD) and complex refractive index (CRI) is required. In this study, we employed the sub-mode VSD and CRI in Chengdu based on the three years observation data to investigate the sub-mode characteristics and climate effects. The annual average fraction of the fine-mode aerosol optical depth (AODf) is 92%, which has the same monthly tendency as the total AOD. But the coarse-mode aerosol optical depth (AODc) has little variation in different months. There are four distinguishing modes of VSD in Chengdu; the median radii are 0.17 μm ± 0.05, 0.31 μm ± 0.12, 1.62 μm ± 0.45, 3.25 μm ± 0.99, respectively. The multi-year average and seasonal variations of fine- and coarse-mode VSD and CRI are also analyzed to characterize aerosols over this region. The fine-mode single scattering albedos (SSAs) are higher than the coarse-mode ones, which suggests that the coarse-mode aerosols have a stronger absorbing effect on solar light than the small-size aerosol particles in Chengdu.

Intra-annual variations of regional aerosol optical depth, vertical distribution, and particle types from multiple satellite and ground-based observational datasets.

The climatic and health effects of aerosols are strongly dependent on the intra-annual variations in their loading and properties. While the seasonal variations of regional aerosol optical depth (AOD) have been extensively studied, understanding the temporal variations in aerosol vertical distribution and particle types is also important for an accurate estimate of aerosol climatic effects. In this paper, we combine the observations from four satellite-borne sensors and several ground-based networks to investigate the seasonal variations of aerosol column loading, vertical distribution, and particle types over three populous regions: the Eastern United States (EUS), Western Europe (WEU), and Eastern and Central China (ECC). In all three regions, column AOD, as well as AOD at heights above 800 m, peaks in summer/spring, probably due to accelerated formation of secondary aerosols and hygroscopic growth. In contrast, AOD below 800m peaks in winter over WEU and ECC regions because more aerosols are confined to lower heights due to the weaker vertical mixing. In the EUS region, AOD below 800m shows two maximums, one in summer and the other in winter. The temporal trends in low-level AOD are consistent with those in surface fine particle (PM2.5) concentrations. AOD due to fine particles (< 0.7 μm diameter) is much larger in spring/summer than in winter over all three regions. However, the coarse mode AOD (> 1.4 μm diameter), generally shows small variability, except that a peak occurs in spring in the ECC region due to the prevalence of airborne dust during this season. When aerosols are classified according to sources, the dominant type is associated with anthropogenic air pollution, which has a similar seasonal pattern as total AOD. Dust and sea-spray aerosols in the WEU region peak in summer and winter, respectively, but do not show an obvious seasonal pattern in the EUS region. Smoke aerosols, as well as absorbing aerosols, present an obvious unimodal distribution with a maximum occurring in summer over the EUS and WEU regions, whereas they follow a bimodal distribution with peaks in August and March (due to crop residue burning) over the ECC region.