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A total of 16 global chemistry transport models and general circulation models have participated in this study; 14 models have been evaluated with regard to their ability to reproduce the near-surface observed number concentration of aerosol particles and cloud condensation nuclei (CCN), as well as derived cloud droplet number concentration (CDNC). Model results for the period 2011-2015 are compared with aerosol measurements (aerosol particle number, CCN and aerosol particle composition in the submicron fraction) from nine surface stations located in Europe and Japan. The evaluation focuses on the ability of models to simulate the average across time state in diverse environments and on the seasonal and short-term variability in the aerosol properties. There is no single model that systematically performs best across all environments represented by the observations. Models tend to underestimate the observed aerosol particle and CCN number concentrations, with average normalized mean bias (NMB) of all models and for all stations, where data are available, of -24% and -35% for particles with dry diameters > 50 and > 120nm, as well as -36% and -34% for CCN at supersaturations of 0.2% and 1.0%, respectively. However, they seem to behave differently for particles activating at very low supersaturations (< 0.1%) than at higher ones. A total of 15 models have been used to produce ensemble annual median distributions of relevant parameters. The model diversity (defined as the ratio of standard deviation to mean) is up to about 3 for simulated N3 (number concentration of particles with dry diameters larger than 3 nm) and up to about 1 for simulated CCN in the extra-polar regions. A global mean reduction of a factor of about 2 is found in the model diversity for CCN at a supersaturation of 0.2% (CCN(0.2)) compared to that for N3, maximizing over regions where new particle formation is important. An additional model has been used to investigate potential causes of model diversity in CCN and bias compared to the observations by performing a perturbed parameter ensemble (PPE) accounting for uncertainties in 26 aerosol-related model input parameters. This PPE suggests that biogenic secondary organic aerosol formation and the hygroscopic properties of the organic material are likely to be the major sources of CCN uncertainty in summer, with dry deposition and cloud processing being dominant in winter. Models capture the relative amplitude of the seasonal variability of the aerosol particle number concentration for all studied particle sizes with available observations (dry diameters larger than 50, 80 and 120nm). The short-term persistence time (on the order of a few days) of CCN concentrations, which is a measure of aerosol dynamic behavior in the models, is underestimated on average by the models by 40% during winter and 20% in summer.

There are few shipborne observations addressing the factors influencing the relationships of the formation and growth of aerosol particles with cloud condensation nuclei (CCN) in remote marine environments. In this study, the physical properties of aerosol particles throughout the Arctic Ocean and Pacific Ocean were measured aboard the Korean icebreaker R/V Araon during the summer of 2017 for 25 d. A number of new particle formation (NPF) events and growth were frequently observed in both Arctic terrestrial and Arctic marine air masses. By striking contrast, NPF events were not detected in Pacific marine air masses. Three major aerosol categories are therefore discussed: (1)  Arctic marine (aerosol number concentration CN2.5: 413±442 cm−3), (2) Arctic terrestrial (CN2.5: 1622±1450 cm−3) and (3) Pacific marine (CN2.5: 397±185 cm−3), following air mass back-trajectory analysis. A major conclusion of this study is not only that the Arctic Ocean is a major source of secondary aerosol formation relative to the Pacific Ocean but also that open-ocean sympagic and terrestrially influenced coastal ecosystems both contribute to shaping aerosol size distributions. We suggest that terrestrial ecosystems – including river outflows and tundra – strongly affect aerosol emissions in the Arctic coastal areas, possibly more than anthropogenic Arctic emissions. The increased river discharge, tundra emissions and melting sea ice should be considered in future Arctic atmospheric composition and climate simulations. The average CCN concentrations at a supersaturation ratios of 0.4 % were 35±40 cm−3, 71±47 cm−3 and 204±87 cm−3 for Arctic marine, Arctic terrestrial and Pacific marine aerosol categories, respectively. Our results aim to help evaluate how anthropogenic and natural atmospheric sources and processes affect the aerosol composition and cloud properties.

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

The seasonal and spatial variations of vertical distribution and optical properties of aerosols over China are studied using long-term satellite observations from the Cloud–Aerosol Lidar with Orthogonal Polarization (CALIOP) and ground-based lidar observations and Aerosol Robotic Network (AERONET) data. The CALIOP products are validated using the ground-based lidar measurements at the Semi-Arid Climate and Environment Observatory of Lanzhou University (SACOL). The Taklamakan Desert and Tibetan Plateau regions exhibit the highest depolarization and color ratios because of the natural dust origin, whereas the North China Plain, Sichuan Basin and Yangtze River Delta show the lowest depolarization and color ratios because of aerosols from secondary formation of the anthropogenic origin. Certain regions, such as the North China Plain in spring and the Loess Plateau in winter, show intermediate depolarization and color ratios because of mixed dust and anthropogenic aerosols. In the Pearl River Delta region, the depolarization and color ratios are similar to but higher than those of the other polluted regions because of combined anthropogenic and marine aerosols. Long-range transport of dust in the middle and upper troposphere in spring is well captured by the CALIOP observations. The seasonal variations in the aerosol vertical distributions reveal efficient transport of aerosols from the atmospheric boundary layer to the free troposphere because of summertime convective mixing. The aerosol extinction lapse rates in autumn and winter are more positive than those in spring and summer, indicating trapped aerosols within the boundary layer because of stabler meteorological conditions. More than 80 % of the column aerosols are distributed within 1.5 km above the ground in winter, when the aerosol extinction lapse rate exhibits a maximum seasonal average in all study regions except for the Tibetan Plateau. The aerosol extinction lapse rates in the polluted regions are higher than those of the less polluted regions, indicating a stabilized atmosphere due to absorptive aerosols in the polluted regions. Our results reveal that the satellite and ground-based remote-sensing measurements provide the key information on the long-term seasonal and spatial variations in the aerosol vertical distribution and optical properties, regional aerosol types, long-range transport and atmospheric stability, which can be utilized to more precisely assess the direct and indirect aerosol effects on weather and climate.

To better understand the aerosol properties over the Arctic, Antarctic and Tibetan Plateau (TP), the aerosol optical properties were investigated using 13 years of CALIPSO (Cloud–Aerosol Lidar and Infrared Pathfinder Satellite Observations) L3 data, and the back trajectories for air masses were also simulated using the Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model. The results show that the aerosol optical depth (AOD) has obvious spatial- and seasonal-variation characteristics, and the aerosol loading over Eurasia, Ross Sea and South Asia is relatively large. The annual-average AODs over the Arctic, Antarctic and TP are 0.046, 0.024 and 0.098, respectively. Seasonally, the AOD values are larger from late autumn to early spring in the Arctic, in winter and spring in the Antarctic, and in spring and summer over the TP. There are no significant temporal trends of AOD anomalies in the three study regions. Clean marine and dust-related aerosols are the dominant types over ocean and land, respectively, in both the Arctic and Antarctic, while dust-related aerosol types have greater occurrence frequency (OF) over the TP. The OF of dust-related and elevated smoke is large for a broad range of heights, indicating that they are likely transported aerosols, while other types of aerosols mainly occurred at heights below 2 km in the Antarctic and Arctic. The maximum OF of dust-related aerosols mainly occurs at 6 km altitude over the TP. The analysis of back trajectories of the air masses shows large differences among different regions and seasons. The Arctic region is more vulnerable to mid-latitude pollutants than the Antarctic region, especially in winter and spring, while the air masses in the TP are mainly from the Iranian Plateau, Tarim Basin and South Asia.

To obtain a thorough knowledge of PM2.5 chemical composition and its impact on aerosol optical properties across China, existing field studies conducted after the year 2000 are reviewed and summarized in terms of geographical, interannual and seasonal distributions. Annual PM2.5 was up to 6 times the National Ambient Air Quality Standards (NAAQS) in some megacities in northern China. Annual PM2.5 was higher in northern than southern cities, and higher in inland than coastal cities. In a few cities with data longer than a decade, PM2.5 showed a slight decrease only in the second half of the past decade, while carbonaceous aerosols decreased, sulfate (SO42-) and ammonium (NH4+) remained at high levels, and nitrate (NO3-) increased. The highest seasonal averages of PM2.5 and its major chemical components were typically observed in the cold seasons. Annual average contributions of secondary inorganic aerosols to PM2.5 ranged from 25 to 48 %, and those of carbonaceous aerosols ranged from 23 to 47 %, both with higher contributions in southern regions due to the frequent dust events in northern China. Source apportionment analysis identified secondary inorganic aerosols, coal combustion and traffic emission as the top three source factors contributing to PM2.5 mass in most Chinese cities, and the sum of these three source factors explained 44 to 82 % of PM2.5 mass on annual average across China. Biomass emission in most cities, industrial emission in industrial cities, dust emission in northern cities and ship emission in coastal cities are other major source factors, each of which contributed 7–27 % to PM2.5 mass in applicable cities.The geographical pattern of scattering coefficient (bsp) was similar to that of PM2.5, and that of aerosol absorption coefficient (bap) was determined by elemental carbon (EC) mass concentration and its coating. bsp in ambient condition of relative humidity (RH) = 80 % can be amplified by about 1.8 times that under dry conditions. Secondary inorganic aerosols accounted for about 60 % of aerosol extinction coefficient (bext) at RH greater than 70 %. The mass scattering efficiency (MSE) of PM2.5 ranged from 3.0 to 5.0 m2 g-1 for aerosols produced from anthropogenic emissions and from 0.7 to 1.0 m2 g-1 for natural dust aerosols. The mass absorption efficiency (MAE) of EC ranged from 6.5 to 12.4 m2 g-1 in urban environments, but the MAE of water-soluble organic carbon was only 0.05 to 0.11 m2 g-1. Historical emission control policies in China and their effectiveness were discussed based on available chemically resolved PM2.5 data, which provides the much needed knowledge for guiding future studies and emissions policies.

The Beijing Climate Center Earth System Model version 1 (BCC-ESM1) is the first version of a fully coupled Earth system model with interactive atmospheric chemistry and aerosols developed by the Beijing Climate Center, China Meteorological Administration. Major aerosol species (including sulfate, organic carbon, black carbon, dust, and sea salt) and greenhouse gases are interactively simulated with a whole panoply of processes controlling emission, transport, gas-phase chemical reactions, secondary aerosol formation, gravitational settling, dry deposition, and wet scavenging by clouds and precipitation. Effects of aerosols on radiation, cloud, and precipitation are fully treated. The performance of BCC-ESM1 in simulating aerosols and their optical properties is comprehensively evaluated as required by the Aerosol Chemistry Model Intercomparison Project (AerChemMIP), covering the preindustrial mean state and time evolution from 1850 to 2014. The simulated aerosols from BCC-ESM1 are quite coherent with Coupled Model Intercomparison Project Phase 5 (CMIP5)-recommended data, in situ measurements from surface networks (such as IMPROVE in the US and EMEP in Europe), and aircraft observations. A comparison of modeled aerosol optical depth (AOD) at 550 nm with satellite observations retrieved from the Moderate Resolution Imaging Spectroradiometer (MODIS) and the Multi-angle Imaging SpectroRadiometer (MISR) and surface AOD observations from the AErosol RObotic NETwork (AERONET) shows reasonable agreement between simulated and observed AOD. However, BCC-ESM1 shows weaker upward transport of aerosols from the surface to the middle and upper troposphere, likely reflecting the deficiency of representing deep convective transport of chemical species in BCC-ESM1. With an overall good agreement between BCC-ESM1 simulated and observed aerosol properties, it demonstrates a success of the implementation of interactive aerosol and atmospheric chemistry in BCC-ESM1.

Proven by multiple theoretical and practical studies, multi-angular spectral polarimetry is ideal for comprehensive retrieval of properties of aerosols. Furthermore, a large number of advanced space polarimeters have been launched recently or planned to be deployed in the coming few years (Dubovik et al., 2019). Nevertheless, at present, practical utilization of aerosol products from polarimetry is rather limited, due to the relatively small number of polarimetric compared to photometric observations, as well as challenges in making full use of the extensive information content available in these complex observations. Indeed, while in recent years several new algorithms have been developed to provide enhanced aerosol retrievals from satellite polarimetry, the practical value of available aerosol products from polarimeters yet remains to be proven. In this regard, this paper presents the analysis of aerosol products obtained by the Generalized Retrieval of Atmosphere and Surface Properties (GRASP) algorithm from POLDER/PARASOL observations. After about a decade of development, GRASP has been adapted for operational processing of polarimetric satellite observations and several aerosol products from POLDER/PARASOL observations have been released. These updated PARASOL/GRASP products are publicly available (e.g., http://www.icare.univ-lille.fr, last access: 16 October 2018, http://www.grasp-open.com/products/, last access: 28 March 2020); the dataset used in the current study is registered under https://doi.org/10.5281/zenodo.3887265 (Chen et al., 2020). The objective of this study is to comprehensively evaluate the GRASP aerosol products obtained from POLDER/PARASOL observations. First, the validation of the entire 2005–2013 archive was conducted by comparing to ground-based Aerosol Robotic Network (AERONET) data. The subjects of the validation are spectral aerosol optical depth (AOD), aerosol absorption optical depth (AAOD) and single-scattering albedo (SSA) at six wavelengths, as well as Ångström exponent (AE), fine-mode AOD (AODF) and coarse-mode AOD (AODC) interpolated to the reference wavelength 550 nm. Second, an inter-comparison of PARASOL/GRASP products with the PARASOL/Operational, MODIS Dark Target (DT), Deep Blue (DB) and Multi-Angle Implementation of Atmospheric Correction (MAIAC) aerosol products for the year 2008 was performed. Over land both satellite data validations and inter-comparisons were conducted separately for different surface types, discriminated by bins of normalized difference vegetation index (NDVI): < 0.2, 0.2 ≤ and < 0.4, 0.4 ≤ and < 0.6, and ≥ 0.6. Three PARASOL/GRASP products were analyzed: GRASP/HP (“High Precision”), Optimized and Models. These different products are consistent but were obtained using different assumptions in aerosol modeling with different accuracies of atmospheric radiative transfer (RT) calculations. Specifically, when using GRASP/HP or Optimized there is direct retrieval of the aerosol size distribution and spectral complex index of refraction. When using GRASP/Models, the aerosol is approximated by a mixture of several prescribed aerosol components, each with their own fixed size distribution and optical properties, and only the concentrations of those components are retrieved. GRASP/HP employs the most accurate RT calculations, while GRASP/Optimized and GRASP/Models are optimized to achieve the best trade-off between accuracy and speed. In all these three options, the underlying surface reflectance is retrieved simultaneously with the aerosol properties, and the radiative transfer calculations are performed “online” during the retrieval. All validation results obtained for the full archive of PARASOL/GRASP products show solid quality of retrieved aerosol characteristics. The GRASP/Models retrievals, however, provided the most solid AOD products, e.g., AOD (550 nm) is unbiased and has the highest correlation (R ∼ 0.92) and the highest fraction of retrievals (∼ 55.3 %) satisfying the accuracy requirements of the Global Climate Observing System (GCOS) when compared to AERONET observations. GRASP/HP and GRASP/Optimized AOD products show a non-negligible positive bias (∼ 0.07) when AOD is low (< 0.2). On the other hand, the detailed aerosol microphysical characteristics (AE, AODF, AODC, SSA, etc.) provided by GRASP/HP and GRASP/Optimized correlate generally better with AERONET than do the results of GRASP/Models. Overall, GRASP/HP processing demonstrates the high quality of microphysical characteristics retrieval versus AERONET. Evidently, the GRASP/Models approach is more adapted for retrieval of total AOD, while the detailed aerosol microphysical properties are limited when a mixture of aerosol models with fixed optical properties are used. The results of a comparative analysis of PARASOL/GRASP and MODIS products showed that, based on validation against AERONET, the PARASOL/GRASP AOD (550 nm) product is of similar and sometimes of higher quality compared to the MODIS products. All AOD retrievals are more accurate and in good agreement over ocean. Over land, especially over bright surfaces, the retrieval quality degrades and the differences in total AOD products increase. The detailed aerosol characteristics, such as AE, AODF and AODC from PARASOL/GRASP, are generally more reliable, especially over land. The global inter-comparisons of PARASOL/GRASP versus MODIS showed rather robust agreement, though some patterns and tendencies were observed. Over ocean, PARASOL/Models and MODIS/DT AOD agree well with the correlation coefficient of 0.92. Over land, the correlation between PARASOL/Models and the different MODIS products is lower, ranging from 0.76 to 0.85. There is no significant global offset; though over bright surfaces MODIS products tend to show higher values compared to PARASOL/Models when AOD is low and smaller values for moderate and high AODs. Seasonal AOD means suggest that PARASOL/GRASP products show more biomass burning aerosol loading in central Africa and dust over the Taklamakan Desert, but less AOD in the northern Sahara. It is noticeable also that the correlation for the data over AERONET sites are somewhat higher, suggesting that the retrieval assumptions generally work better over AERONET sites than over the rest of the globe. One of the potential reasons may be that MODIS retrievals, in general, rely more on AERONET climatology than GRASP retrievals. Overall, the analysis shows that the quality of AOD retrieval from multi-angular polarimetric observations like POLDER is at least comparable to that of single-viewing MODIS-like imagers. At the same time, the multi-angular polarimetric observations provide more information on other aerosol properties (e.g., spectral AODF, AODC, AE), as well as additional parameters such as AAOD and SSA.