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This study focuses on the characterization of aerosol hygroscopicity using remote sensing techniques. We employ a Mie–Raman–fluorescence lidar (Lille Lidar for Atmospheric Study, LILAS), developed at the ATOLL platform, Laboratoire d'Optique Atmosphérique, Lille, France, in combination with the RPG-HATPRO-G5 microwave radiometer to enable continuous aerosol and water vapor monitoring. We identify hygroscopic growth cases when an aerosol layer exhibits an increase in both aerosol backscattering coefficient and relative humidity. By examining the fluorescence backscattering coefficient, which remains unaffected by the presence of water vapor, the potential temperature, and the absolute humidity, we verify the homogeneity of the aerosol layer. Consequently, the change in the backscattering coefficient is solely attributed to water uptake. The Hänel theory is employed to describe the evolution of the backscattering coefficient with relative humidity and introduces a hygroscopic coefficient, γ , which depends on the aerosol type. The particularity of this method revolves around the use of the fluorescence which is employed to take into account and correct the aerosol concentration variations in the layer. Case studies conducted on 29 July and 9 March 2021 examine, respectively, an urban and a smoke aerosol layer. For the urban case, γ is estimated as 0.47 ± 0.03 at 532 nm; as for the smoke case, the estimation of γ is 0.5 ± 0.3. These values align with those reported in the literature for urban and smoke particles. Our findings highlight the efficiency of the Mie–Raman–fluorescence lidar and microwave radiometer synergy in characterizing aerosol hygroscopicity. The results contribute to advance our understanding of atmospheric processes, aerosol–cloud interactions, and climate modeling. [ABSTRACT FROM AUTHOR]

We present the capabilities of a compact dual-wavelength depolarization lidar to assess the spatiotemporal variations in aerosol properties aboard moving vectors. Our approach involves coupling the lightweight Cimel CE376 lidar, which provides measurements at 532 and 808 nm and depolarization at 532 nm , with a photometer to monitor aerosol properties. The assessments, both algorithmic and instrumental, were conducted at ATOLL (ATmospheric Observatory of LiLle) platform operated by the Laboratoire d'Optique Atmosphérique (LOA), in Lille, France. An early version of the CE376 lidar co-located with the CE318-T photometer and with a multi-wavelength Raman lidar were considered for comparisons and validation. We developed a modified Klett inversion method for simultaneous two-wavelength elastic lidar and photometer measurements. Using this setup, we characterized aerosols during two distinct events of Saharan dust and dust smoke aerosols transported over Lille in spring 2021 and summer 2022. For validation purposes, comparisons against the Raman lidar were performed, demonstrating good agreement in aerosol properties with relative differences of up to 12 % in the depolarization measurements. Moreover, a first dataset of CE376 lidar and photometer performing on-road measurements was obtained during the FIREX-AQ (Fire Influence on Regional to Global Environments and Air Quality) field campaign deployed in summer 2019 over the northwestern USA. By lidar and photometer mapping in 3D, we investigated the transport of released smoke from active fire spots at William Flats (northeast WA, USA). Despite extreme environmental conditions, our study enabled the investigation of aerosol optical properties near the fire source, distinguishing the influence of diffuse, convective, and residual smoke. Backscatter, extinction profiles, and column-integrated lidar ratios at 532 and 808 nm were derived for a quality-assured dataset. Additionally, the extinction Ångström exponent (EAE), color ratio (CR), attenuated color ratio (ACR), and particle linear depolarization ratio (PLDR) were derived. In this study, we discuss the capabilities (and limitations) of the CE376 lidar in bridging observational gaps in aerosol monitoring, providing valuable insights for future research in this field. [ABSTRACT FROM AUTHOR]

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 10.5281/zenodo.6395384 (Li et al., 2022b). [ABSTRACT FROM AUTHOR]

The study presents a climatology of aerosol composition concentration obtained by a recently developed GRASP/Component (GRASP stands for the Generalized Retrieval of Atmosphere and Surface Properties algorithm) approach applied to the whole archive of POLDER-3 observations. The conceptual specific of the GRASP/Component approach is in direct retrieval of aerosol speciation (component fraction) without an intermediate retrievals of aerosol optical characteristics. Despite 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 and dust components with those of the MERRA-2 (Modern-Era Retrospective Analysis for Research and Applications, version 2) product. Quite reasonable general agreement in spatial and temporal distribution of the species provided by GRASP and MERRA-2 was found, 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 concentration of absorbing (black carbon, brown carbon, iron oxides content in mineral dust) and scattering (ammonium sulphate and nitrate, organic carbon, non-absorbing dust) aerosol, represent scarce but imperative information for validation and potential adjustment of chemical transport models. The aerosol optical properties derived by GRASP/Component were found to agree well with the AERONET ground reference data and fully consistent with the previous GRASP Optimized, High Precision 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 inside about aerosol distributions and, therefore, demonstrates advantages of multi-angular polarimetric satellite observations as the next frontier for aerosol inversion from advanced satellite observations. [ABSTRACT FROM AUTHOR]

Aerosol absorption is a key property to assess the radiative impacts of aerosols on climate at both global and regional scales. The aerosol physico-chemical and optical properties remain not sufficiently constrained in climate models, with difficulties to properly represent both the aerosol load and their absorption properties in clear and cloudy scenes, especially for absorbing biomass burning aerosols (BBA). In this study we focus on biomass burning (BB) particle plumes transported above clouds over the southeast Atlantic (SEA) region off the southwest coast of Africa, in order to improve the representation of their physico-chemical and absorption properties. The methodology is based on aerosol regional numerical simulations from the WRF-Chem coupled meteorology–chemistry model combined with a detailed inventory of BB emissions and various sets of innovative aerosol remote sensing observations, both in clear and cloudy skies from the POLDER-3/PARASOL space sensor. Current literature indicates that some organic aerosol compounds (OC), called brown carbon (BrOC), primarily emitted by biomass combustion absorb the ultraviolet-blue radiation more efficiently than pure black carbon (BC). We exploit this specificity by comparing the spectral dependence of the aerosol single scattering albedo (SSA) derived from the POLDER-3 satellite observations in the 443–1020 nm wavelength range with the SSA simulated for different proportions of BC, OC and BrOC at the source level, considering the homogeneous internal mixing state of particles. These numerical simulation experiments are based on two main constraints: maintaining a realistic aerosol optical depth both in clear and above cloudy scenes and a realistic BC/OC mass ratio. Modelling experiments are presented and discussed to link the chemical composition with the absorption properties of BBA and to provide estimates of the relative proportions of black, organic and brown carbon in the African BBA plumes transported over the SEA region for July 2008. The absorbing fraction of organic aerosols in the BBA plumes, i.e. BrOC, is estimated at 2 % to 3 %. The simulated mean SSA are 0.81 (565 nm) and 0.84 (550 nm) in clear and above cloudy scenes respectively, in good agreement with those retrieved by POLDER-3 (0.85±0.05 at 565 nm in clear sky and at 550 nm above clouds) for the studied period. [ABSTRACT FROM AUTHOR]

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 & 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, AOD F , and AOD C , respectively), Ångström exponent (AE), and the spherical/non-spherical partition of the coarse-mode AOD (AOD CS and AOD CNS , 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 > 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 AOD F (- 0.0020 yr -1 at 865 nm) than for AOD C. Our analysis also suggests that the North Atlantic Oscillation (NAO) index explains a significant part of the interannual variability of POLDER-3 AOD C , 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 AOD F-865 nm<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. [ABSTRACT FROM AUTHOR]

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 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. [ABSTRACT FROM AUTHOR]

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 amount of polarimetric observations 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, www.grasp-open.com/products/), 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 6 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 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 options, the underlying surface reflectance is retrieved simultaneously with the aerosol properties and the radiative transfer calculations are performed on line 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, 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 and 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, 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 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 is 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 those 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. [ABSTRACT FROM AUTHOR]

We invert global black carbon (BC), organic carbon (OC) and desert dust (DD) aerosol emissions from POLDER/PARASOL spectral aerosol optical depth (AOD) and aerosol absorption optical depth (AAOD) using the GEOS-Chem inverse modeling framework. Our inverse modeling framework uses standard a priori emissions to provide a posteriori emissions that are constrained by POLDER/PARASOL AODs and AAODs. The following global emission values were retrieved for the three aerosol components: 18.4 Tg yr -1 for BC, 109.9 Tg yr -1 for OC and 731.6 Tg yr -1 for DD for the year 2010. These values show a difference of +166.7 %, + 184.0 % and -42.4 %, respectively, with respect to the a priori values of emission inventories used in "standard" GEOS-Chem runs. The model simulations using a posteriori emissions (i.e., retrieved emissions) provide values of 0.119 for global mean AOD and 0.0071 for AAOD at 550 nm, which are +13.3 % and +82.1 %, respectively, higher than the AOD and AAOD obtained using the a priori values of emissions. Additionally, the a posteriori model simulation of AOD, AAOD, single scattering albedo, Ångström exponent and absorption Ångström exponent show better agreement with independent AERONET, MODIS and OMI measurements than the a priori simulation. Thus, this study suggests that using satellite-constrained global aerosol emissions in aerosol transport models can improve the accuracy of simulated global aerosol properties. [ABSTRACT FROM AUTHOR]

This study presents a novel methodology for the remote monitoring of aerosol components over large spatial and temporal domains. The concept is realized within the GRASP (Generalized Retrieval of Aerosol and Surface Properties) algorithm to directly infer aerosol components from the measured radiances. The observed aerosols are assumed to be mixtures of hydrated soluble particles embedded with black carbon, brown carbon, iron oxide, and other (non-absorbing) insoluble inclusions. The complex refractive indices of the dry components are fixed a priori (although the refractive index of the soluble host is allowed to vary with hydration), and the complex refractive indices of the mixture are computed using mixing rules. The volume fractions of these components are derived along with the size distribution and the fraction of spherical particles, as well as the spectral surface reflectance in cases when the satellite data are inverted. The retrieval is implemented as a statistically optimized fit in a continuous space of solutions. This contrasts with most conventional approaches in which the type of aerosol is either associated with a pre-assumed aerosol model that is included in a set of look-up tables, or determined from the analysis of the retrieved aerosol optical parameters (e.g., single scattering albedo, refractive index, among others, provided by the AERONET retrieval algorithm); here, we retrieve the aerosol components explicitly. The approach also bridges directly to the quantities used in global chemical transport models. We first tested the approach with synthetic data to estimate the uncertainty, and then applied it to real ground-based AERONET and spaceborne POLDER/PARASOL observations; thus, the study presents a first attempt to derive aerosol components from satellite observations specifically tied to global chemical transport model quantities. Our results indicate aerosol optical characteristics that are highly consistent with standard products (e.g., R of ∼0.9 for aerosol optical thickness) and demonstrate an ability to separate intrinsic optical properties of fine- and coarse-sized aerosols. We applied our method to POLDER/PARASOL radiances on the global scale and obtained spatial and temporal patterns of the aerosol components that agree well with existing knowledge on aerosol sources and transport features. Finally, we discuss limitations and perspectives of this new technique. [ABSTRACT FROM AUTHOR]

Spatio-Temporal Variability of Aerosol Components, Their Optical and Microphysical Properties over North China during Winter Haze in 2012, as Derived from POLDER/PARASOL Satellite Observations. In the published article [[1]], there was an error regarding the affiliation for Yang Ou, Zhengqiang Li, and Ying Zhang. Footnotes 1 B Disclaimer/Publisher's Note: b The statements, opinions and data contained in all publications are solely those of the individual author(s) and contributor(s) and not of MDPI and/or the editor(s). [Extracted from the article]

Pollution haze is a frequent phenomenon in the North China Plain (NCP) appearing during winter when the aerosol is affected by various pollutant sources and has complex distribution of the aerosol properties, while different aerosol components may have various critical effects on air quality, human health and radiative balance. Therefore, large-scale and accurate aerosol components characterization is urgently and highly desirable but hardly achievable at the regional scale. In this respect, directional and polarimetric remote sensing observations have great potential for providing information about the aerosol components. In this study, a state-of-the-art GRASP/Component approach was employed for attempting to characterize aerosol components in the NCP using POLDER/PARASOL satellite observations. The analysis was done for January 2012 in Beijing (BJ) and Shanxi (SX). The results indicate a peak of the BC mass concentration in an atmospheric column of 82.8 mg/m2 in the SX region, with a mean of 29.2 mg/m2 that is about four times higher than one in BJ (8.9 mg/m2). The mean BrC mass concentrations are, however, higher in BJ (up to ca. 271 mg/m2) than that in SX, which can be attributed to a higher anthropogenic emission. The mean amount of fine ammonium sulfate-like particles observed in the BJ region was three times lower than in SX (131 mg/m2). The study also analyzes meteorological and air quality data for characterizing the pollution event in BJ. During the haze episode, the results suggest a rapid increase in the fine mode aerosol volume concentration associated with a decrease of a scale height of aerosol down to 1500 m. As expected, the values of aerosol optical depth (AOD), absorbing aerosol optical depth (AAOD) and fine mode aerosol optical depth (AODf) are much higher on hazy days. The mass fraction of ammonium sulfate-like aerosol increases from about 13% to 29% and mass concentration increases from 300 mg/m2 to 500 mg/m2. The daily mean PM2.5 concentration and RH independently measured during these reported pollution episodes reach up to 425 g/m3 and 80% correspondingly. The monthly mean mass concentrations of other aerosol components in the BJ are found to be in agreement with the results of previous research works. Finally, a preliminary comparison of these remote sensing derived results with literature and in situ PM2.5 measurements is also presented. [ABSTRACT FROM AUTHOR]

We have developed a method for evaluating the fidelity of the Aerosol Robotic Network (AERONET) retrieval algorithms by mimicking atmospheric extinction and radiance measurements in a laboratory experiment. This enables radiometric retrievals that use the same sampling volumes, relative humidities, and particle size ranges as observed by other in situ instrumentation in the experiment. We use three Cavity Attenuated Phase Shift (CAPS) monitors for extinction and University of Maryland Baltimore County's (UMBC) three-wavelength Polarized Imaging Nephelometer (PI-Neph) for angular scattering measurements. We subsample the PI-Neph radiance measurements to angles that correspond to AERONET almucantar scans, with simulated solar zenith angles ranging from 50 ∘ to 77 ∘ . These measurements are then used as input to the Generalized Retrieval of Aerosol and Surface Properties (GRASP) algorithm, which retrieves size distributions, complex refractive indices, single-scatter albedos, and bistatic LiDAR ratios for the in situ samples. We obtained retrievals with residuals less than 8% for about 90 samples. Samples were alternately dried or humidified, and size distributions were limited to diameters of less than 1.0 or 2.5 μ m by using a cyclone. The single-scatter albedo at 532 nm for these samples ranged from 0.59 to 1.00 when computed with CAPS extinction and Particle Soot Absorption Photometer (PSAP) absorption measurements. The GRASP retrieval provided single-scatter albedos that are highly correlated with the in situ single-scatter albedos, and the correlation coefficients ranged from 0.916 to 0.976, depending upon the simulated solar zenith angle. The GRASP single-scatter albedos exhibited an average absolute bias of +0.023–0.026 with respect to the extinction and absorption measurements for the entire dataset. We also compared the GRASP size distributions to aerodynamic particle size measurements, using densities and aerodynamic shape factors that produce extinctions consistent with our CAPS measurements. The GRASP effective radii are highly correlated (R = 0.80) and biased under the corrected aerodynamic effective radii by 1.3% (for a simulated solar zenith angle of θ ∘ = 50 ∘ ); the effective variance indicated a correlation of R = 0.51 and a relative bias of 280%. Finally, our apparatus was not capable of measuring backscatter LiDAR ratios, so we measured bistatic LiDAR ratios at a scattering angle of 173 degrees. The GRASP bistatic LiDAR ratios had correlations of 0.71 to 0.86 (depending upon simulated θ ∘ ) with respect to in situ measurements, positive relative biases of 2–10%, and average absolute biases of 1.8–7.9 sr. [ABSTRACT FROM AUTHOR]

MOABAI campaign (Mobile Observations of Atmosphere By vehicle-borne Aerosol measurement Instruments) has been carried out during 5-23 May 2017 in North China Plain, one of the most populated and polluted regions of China, where long-standing heavy aerosol pollution episodes frequently occur. The campaign was purposed to elucidate and quantify the 4-D distribution of aerosols in a polluted region where few aerosol measurements are available, in order to get a comprehensive characterization of aerosol properties and their vertical distribution in variable atmospheric situations and capture signatures of regional transport of aerosols. The measurements were performed using a state-of-the-art instrumented van, including both remote sensing and in situ instrumentation. A CIMEL micropulse lidar and PLASMA mobile sun photometer, performing measurements during motion, were transported and integrated on site in the existing van already equipped with in situ instruments. The in situ instruments consisted of a nephelometer, an aethalometer, a Grimm Sky-OPC and trace gas analyzers for NO2, SO2 and O3. Ten days of mobile measurements have been recorded, six days in Beijing on the 4th, 5th and 6th ring-roads by daytime and nighttime and 4 days outside of Beijing, reaching Baoding, Tianjin and Tangshan. Four types of atmospheric situations were observed: two days of pollution and "background" (moderate pollution) situation in Beijing with a contribution of dust transported from Gobi desert (9 and 11 May), three heavy pollution days, when the air flow moved from south of China (18, 19 and 21 May), one day with moderate pollution (15 May) and one "clean" day, marked by lower aerosol loading (13 May), but with a contribution of long-range transported aerosols in altitude. In the case of pollution days, the PBL extended up to 1 - 1.5 km altitude and marked by high AOD at 440 nm (0.8 - 1.8), highest values being recorded when the air masses were moving from South direction, and Angstrom Exponent (AE) values typical for fine mode particles predominance (1.2 – 1.6). For the "background" and "clean" situations, a contribution of both fine and coarse mode aerosols was evidenced, indicated by lower AE and by transported aerosol layers above 2 km. Three mobile observations were carried out outside Beijing: Beijing – Baoding - Tianjin (16 May), Tianjin - Tangshan (17 May) and Tangshan - Beijing (18 May). The AOD at 440 nm was in the range of 0.2 - 0.7, 0.3 - 0.79 and 0.43 - 1.35 for transects on 16, 17 and 18 May, respectively. The values of AE were in the range of 0.38 - 1.5, 1.02 - 1.9 and 1.22 - 1.74 for 16, 17 and 18 May, respectively. The lidar profiles showed higher particle concentrations when reaching polluted regions of Baoding, Tianjin, Binhai New Area and Tangshan and transport of desert dust from Inner Mongolia at about 2-3 km altitude. Mapping of AOD, Angstrom Exponent and retrieved vertical profiles of aerosol extinction coefficients and column-integrated volume size distribution have been achieved. Results from some case studies in Beijing and along Tianjin coast will be presented. [ABSTRACT FROM AUTHOR]

The western Mediterranean atmosphere is impacted by a variety of aerosol sources, producing a complex and variable mixture of natural and anthropogenic particles, with different chemical and physical properties. Satellite sensors provide a useful global coverage of aerosol parameters but through indirect measurements that request careful validation. Here we present the results of a long-term regional scale analysis of the full dataset (March 2005 and October 2013) of POLDER-3/PARASOL ocean operational retrievals of the total, fine and coarse aerosol optical depth (AOD, AODF and AODC), Angstrom exponent (AE), and the spherical/non-spherical partition of coarse-mode AOD (AODCS and AODCNS), respectively. The evaluation is performed using data from seventeen coastal and insular ground-based AERONET sites on one side, and airborne vertical profiles of aerosol extinction and number size distribution obtained by the SAFIRE ATR 42 aircraft operated in the area during summer 2012 and 2013 campaigns of the MISTRALS/ChArMEx programme on the other side.This study provides the first regional evaluation of uncertainties of the POLDER-3 products, and highlights their quality. The POLDER-3 Ångström exponent, representing AOD spectral dependence in link with the aerosol particle size distribution, is biased towards small values. This bias, however, does not prevent using AE for classifying the regional aerosol laden air masses. AODF corresponds to particles smaller than 0.6-0.8 µm in diameter and appears suitable to monitor the aerosol submicron fraction from space. We also provide an original validation of POLDER-3 AODC and its spherical/non-spherical partition, which shows agreement within 25% with AERONET shape retrievals when the aerosol coarse fraction dominates. This work now serves the dust model validation undergoing in the ERA4CS DustClim project. [ABSTRACT FROM AUTHOR]