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In this study, we developed a novel algorithm based on the collocated Moderate Resolution Imaging Spectroradiometer (MODIS) thermal infrared (TIR) observations and dust vertical profiles from the Cloud–Aerosol Lidar with Orthogonal Polarization (CALIOP) to simultaneously retrieve dust aerosol optical depth at 10 µm (DAOD10 µm) and the coarse-mode dust effective diameter (Deff) over global oceans. The accuracy of the Deff retrieval is assessed by comparing the dust lognormal volume particle size distribution (PSD) corresponding to retrieved Deff with the in situ-measured dust PSDs from the AERosol Properties – Dust (AER-D), Saharan Mineral Dust Experiment (SAMUM-2), and Saharan Aerosol Long-Range Transport and Aerosol–Cloud-Interaction Experiment (SALTRACE) field campaigns through case studies. The new DAOD10 µm retrievals were evaluated first through comparisons with the collocated DAOD10.6 µm retrieved from the combined Imaging Infrared Radiometer (IIR) and CALIOP observations from our previous study (Zheng et al., 2022). The pixel-to-pixel comparison of the two DAOD retrievals indicates a good agreement (R∼0.7) and a significant reduction in (∼50 %) retrieval uncertainties largely thanks to the better constraint on dust size. In a climatological comparison, the seasonal and regional (2∘×5∘) mean DAOD10 µm retrievals based on our combined MODIS and CALIOP method are in good agreement with the two independent Infrared Atmospheric Sounding Interferometer (IASI) products over three dust transport regions (i.e., North Atlantic (NA; R=0.9), Indian Ocean (IO; R=0.8) and North Pacific (NP; R=0.7)). Using the new retrievals from 2013 to 2017, we performed a climatological analysis of coarse-mode dust Deff over global oceans. We found that dust Deff over IO and NP is up to 20 % smaller than that over NA. Over NA in summer, we found a ∼50 % reduction in the number of retrievals with Deff>5 µm from 15 to 35∘ W and a stable trend of Deff average at 4.4 µm from 35∘ W throughout the Caribbean Sea (90∘ W). Over NP in spring, only ∼5 % of retrieved pixels with Deff>5 µm are found from 150 to 180∘ E, while the mean Deff remains stable at 4.0 µm throughout eastern NP. To the best of our knowledge, this study is the first to retrieve both DAOD and coarse-mode dust particle size over global oceans for multiple years. This retrieval dataset provides insightful information for evaluating dust longwave radiative effects and coarse-mode dust particle size in models.

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).

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.

Measurements performed in western Africa (Senegal) during the SHADOW field campaign are analyzed to show that spectral dependence of the imaginary part of the complex refractive index (CRI) of dust can be revealed by lidar-measured particle parameters. Observations in April 2015 provide good opportunity for such study, because, due to high optical depth of the dust, exceeding 0.5, the extinction coefficient could be derived from lidar measurements with high accuracy and the contribution of other aerosol types, such as biomass burning, was negligible. For instance, in the second half of April 2015, AERONET observations demonstrated a temporal decrease in the imaginary part of the CRI at 440 nm from approximately 0.0045 to 0.0025. This decrease is in line with a change in the relationship between the lidar ratios (the extinction-to-backscattering ratio) at 355 and 532 nm (S355 and S532). For instance in the first half of April, S355∕S532 is as high as 1.5 and the backscatter Ångström exponent, Aβ, is as low as −0.75, while after 15 April S355/S532=1.0 and Aβ is close to zero. The aerosol depolarization ratio δ532 for the whole of April exceeded 30 % in the height range considered, implying that no other aerosol, except dust, occurred. The performed modeling confirmed that the observed S355∕S532 and Aβ values match the spectrally dependent imaginary part of the refractive index as can be expected for mineral dust containing iron oxides. The second phase of the SHADOW campaign was focused on evaluation of the lidar ratio of smoke and estimates of its dependence on relative humidity (RH). For five studied smoke episodes the lidar ratio increases from 44±5 to 66±7 sr at 532 nm and from 62±6 to 80±8 sr at 355 nm, when RH varied from 25 % to 85 %. Performed numerical simulations demonstrate that observed ratio S355∕S532, exceeding 1.0 in the smoke plumes, can indicate an increase in the imaginary part of the smoke particles in the ultraviolet (UV) range.

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.

Chemical composition, microphysical, and optical properties of atmospheric aerosol deep inland in the Negev Desert of Israel are found to be influenced by daily occurrences of sea breeze flow from the Mediterranean Sea. Abrupt increases in aerosol volume concentration and shifts of size distributions towards larger sizes, which are associated with increase in wind speed and atmospheric water content, were systematically recorded during the summertime at a distance of at least 80 km from the coast. Chemical imaging of aerosol samples showed an increased contribution of highly hygroscopic particles during the intrusion of the sea breeze. Besides a significant fraction of marine aerosols, the amount of internally mixed marine and mineral dust particles was also increased during the sea breeze period. The number fraction of marine and internally mixed particles during the sea breeze reached up to 88 % in the PM1–2. 5 and up to 62 % in the PM2. 5–10 size range. Additionally, numerous particles with residuals of liquid coating were observed by SEM/EDX analysis. Ca-rich dust particles that had reacted with anthropogenic nitrates were evidenced by Raman microspectroscopy. The resulting hygroscopic particles can deliquesce at very low relative humidity. Our observations suggest that aerosol hygroscopic growth in the Negev Desert is induced by the daily sea breeze arrival. The varying aerosol microphysical and optical characteristics perturb the solar and thermal infrared radiations. The changes in aerosol properties induced by the sea breeze, relative to the background situation, doubled the shortwave radiative cooling at the surface (from −10 to −20.5 W m−2) and increased by almost 3 times the warming of the atmosphere (from 5 to 14 W m−2), as evaluated for a case study. Given the important value of observed liquid coating of particles, we also examined the possible influence of the particle homogeneity assumption on the retrieval of aerosol microphysical characteristics. The tests suggest that sensitivity to the coating appears if backward scattering and polarimetric measurements are available for the inversion algorithm. This may have an important implication for retrievals of aerosol microphysical properties in remote sensing applications.

West Africa and the adjacent oceanic regions are very important locations for studying dust properties and their influence on weather and climate. The SHADOW (study of SaHAran Dust Over West Africa) campaign is performing a multiscale and multilaboratory study of aerosol properties and dynamics using a set of in situ and remote sensing instruments at an observation site located at the IRD (Institute for Research and Development) in Mbour, Senegal (14° N, 17° W). In this paper, we present the results of lidar measurements performed during the first phase of SHADOW (study of SaHAran Dust Over West Africa) which occurred in March–April 2015. The multiwavelength Mie–Raman lidar acquired 3β + 2α + 1δ measurements during this period. This set of measurements has permitted particle-intensive properties, such as extinction and backscattering Ångström exponents (BAE) for 355/532 nm wavelengths' corresponding lidar ratios and depolarization ratio at 532 nm, to be determined. The mean values of dust lidar ratios during the observation period were about 53 sr at both 532 and 355 nm, which agrees with the values observed during the SAMUM-1 and SAMUM-2 campaigns held in Morocco and Cabo Verde in 2006 and 2008. The mean value of the particle depolarization ratio at 532 nm was 30 ± 4.5 %; however, during strong dust episodes this ratio increased to 35 ± 5 %, which is also in agreement with the results of the SAMUM campaigns. The backscattering Ångström exponent during the dust episodes decreased to ∼ −0.7, while the extinction Ångström exponent, though negative, was greater than −0.2. Low values of BAE can likely be explained by an increase in the imaginary part of the dust refractive index at 355 nm compared to 532 nm. The dust extinction and backscattering coefficients at multiple wavelengths were inverted to the particle microphysics using the regularization algorithm and the model of randomly oriented spheroids. The analysis performed has demonstrated that the spectral dependence of the imaginary part of the dust refractive index may significantly influence the inversion results and should be taken into account.

The evaluation of aerosol radiative effect on broadband hemispherical solar flux is often performed using simplified spectral and directional scattering characteristics of atmospheric aerosol and underlying surface reflectance. In this study we present a rigorous yet fast computational tool that accurately accounts for detailed variability of both spectral and angular scattering properties of aerosol and surface reflectance in calculation of direct aerosol radiative effect. The tool is developed as part of the GRASP (Generalized Retrieval of Aerosol and Surface Properties) project. We use the tool to evaluate instantaneous and daily average radiative efficiencies (radiative effect per unit aerosol optical thickness) of several key atmospheric aerosol models over different surface types. We then examine the differences due to neglect of surface reflectance anisotropy, nonsphericity of aerosol particle shape and accounting only for aerosol angular scattering asymmetry instead of using full phase function. For example, it is shown that neglecting aerosol particle nonsphericity causes mainly overestimation of the aerosol cooling effect and that magnitude of this overestimate changes significantly as a function of solar zenith angle (SZA) if the asymmetry parameter is used instead of detailed phase function. It was also found that the nonspherical–spherical differences in the calculated aerosol radiative effect are not modified significantly if detailed BRDF (bidirectional reflectance distribution function) is used instead of Lambertian approximation of surface reflectance. Additionally, calculations show that usage of only angular scattering asymmetry, even for the case of spherical aerosols, modifies the dependence of instantaneous aerosol radiative effect on SZA. This effect can be canceled for daily average values, but only if sun reaches the zenith; otherwise a systematic bias remains. Since the daily average radiative effect is obtained by integration over a range of SZAs, the errors vary with latitude and season. In summary, the present analysis showed that use of simplified assumptions causes systematic biases, rather than random uncertainties, in calculation of both instantaneous and daily average aerosol radiative effect. Finally, we illustrate application of the rigorous aerosol radiative effect calculations performed as part of GRASP aerosol retrieval from real POLDER/PARASOL satellite observations.

The Chemistry-Aerosol Mediterranean Experiment (ChArMEx; http://charmex.lsce.ipsl.fr) is a collaborative research program federating international activities to investigate Mediterranean regional chemistry-climate interactions. A special observing period (SOP-1a) including intensive airborne measurements was performed in the framework of the Aerosol Direct Radiative Impact on the regional climate in the MEDiterranean region (ADRIMED) project during the Mediterranean dry season over the western and central Mediterranean basins, with a focus on aerosol-radiation measurements and their modeling. The SOP-1a took place from 11 June to 5 July 2013. Airborne measurements were made by both the ATR-42 and F-20 French research aircraft operated from Sardinia (Italy) and instrumented for in situ and remote-sensing measurements, respectively, and by sounding and drifting balloons, launched in Minorca. The experimental setup also involved several ground-based measurement sites on islands including two ground-based reference stations in Corsica and Lampedusa and secondary monitoring sites in Minorca and Sicily. Additional measurements including lidar profiling were also performed on alert during aircraft operations at EARLINET/ACTRIS stations at Granada and Barcelona in Spain, and in southern Italy. Remote-sensing aerosol products from satellites (MSG/SEVIRI, MODIS) and from the AERONET/PHOTONS network were also used. Dedicated meso-scale and regional modeling experiments were performed in relation to this observational effort. We provide here an overview of the different surface and aircraft observations deployed during the ChArMEx/ADRIMED period and of associated modeling studies together with an analysis of the synoptic conditions that determined the aerosol emission and transport. Meteorological conditions observed during this campaign (moderate temperatures and southern flows) were not favorable to producing high levels of atmospheric pollutants or intense biomass burning events in the region. However, numerous mineral dust plumes were observed during the campaign, with the main sources located in Morocco, Algeria and Tunisia, leading to aerosol optical depth (AOD) values ranging between 0.2 and 0.6 (at 440 nm) over the western and central Mediterranean basins. One important point of this experiment concerns the direct observations of aerosol extinction onboard the ATR-42, using the CAPS system, showing local maxima reaching up to 150 M m−1 within the dust plume. Non-negligible aerosol extinction (about 50 M m−1) has also been observed within the marine boundary layer (MBL). By combining the ATR-42 extinction coefficient observations with absorption and scattering measurements, we performed a complete optical closure revealing excellent agreement with estimated optical properties. This additional information on extinction properties has allowed calculation of the dust single scattering albedo (SSA) with a high level of confidence over the western Mediterranean. Our results show a moderate variability from 0.90 to 1.00 (at 530 nm) for all flights studied compared to that reported in the literature on this optical parameter. Our results underline also a relatively low difference in SSA with values derived near dust sources. In parallel, active remote-sensing observations from the surface and onboard the F-20 aircraft suggest a complex vertical structure of particles and distinct aerosol layers with sea spray and pollution located within the MBL, and mineral dust and/or aged North American smoke particles located above (up to 6–7 km in altitude). Aircraft and balloon-borne observations allow one to investigate the vertical structure of the aerosol size distribution showing particles characterized by a large size (> 10 µm in diameter) within dust plumes. In most of cases, a coarse mode characterized by an effective diameter ranging between 5 and 10 µm, has been detected above the MBL. In terms of shortwave (SW) direct forcing, in situ surface and aircraft observations have been merged and used as inputs in 1-D radiative transfer codes for calculating the aerosol direct radiative forcing (DRF). Results show significant surface SW instantaneous forcing (up to −90 W m−2 at noon). Aircraft observations provide also original estimates of the vertical structure of SW and LW radiative heating revealing significant instantaneous values of about 5° K per day in the solar spectrum (for a solar angle of 30°) within the dust layer. Associated 3-D modeling studies from regional climate (RCM) and chemistry transport (CTM) models indicate a relatively good agreement for simulated AOD compared with observations from the AERONET/PHOTONS network and satellite data, especially for long-range dust transport. Calculations of the 3-D SW (clear-sky) surface DRF indicate an average of about −10 to −20 W m−2 (for the whole period) over the Mediterranean Sea together with maxima (−50 W m−2) over northern Africa. The top of the atmosphere (TOA) DRF is shown to be highly variable within the domain, due to moderate absorbing properties of dust and changes in the surface albedo. Indeed, 3-D simulations indicate negative forcing over the Mediterranean Sea and Europe and positive forcing over northern Africa. Finally, a multi-year simulation, performed for the 2003 to 2009 period and including an ocean–atmosphere (O–A) coupling, underlines the impact of the aerosol direct radiative forcing on the sea surface temperature, O–A fluxes and the hydrological cycle over the Mediterranean.

Total and polarized radiances provided by the Polarization and Directionality of Earth Reflectances (POLDER) satellite sensor are used to retrieve the microphysical and optical properties of the volcanic plume observed during the Eyjafjallajökull volcano eruption in 2010, over cloud-free and cloudy ocean scenes. We selected two plume conditions, fresh aerosols near the sources (three cases) and a downwind volcanic plume observed over the North Sea 30 h after its injection into the atmosphere (aged aerosols). In the near-source conditions, the aerosol properties depend on the distance to the plume. Within the near-source plume, aerosols are mainly non-spherical and in the coarse mode with an effective radius equal to 1.75 (±0.25) μm and an Ångström exponent (AE) close to 0.0. Far from the plume, in addition to the coarse mode, there are particles retrieved in the accumulation mode, suggesting a mixture of sulfate aerosols and volcanic dust, resulting in an AE around 0.8. The properties of the aerosols also depend on whether the plume is fresh or aged. For the downwind (aged) plume, if non-spherical coarse particles as well as some fine mode particles are retrieved, the AE is higher, around ~0.4. In addition, rather low values for the real part of the refractive index (RR) were retrieved for the fresh plume (1.38 < RR < 1.48). Single scattering albedo (SSA) values ranging between 0.92 and 0.98 were retrieved over some parts of the near-source plume; despite the low accuracy of our retrievals, the derived SSA values suggest that the ash particles are rather absorbing. To consider the particle shape, a combination of spheroid models was used. Although the employed model enabled accurate modeling of the POLDER signal in the case of non-spherical ash, our approach failed to model the signal over the optically thickest parts of the near-source plume. The most probable reason for this is the presence of ice crystals within the plume. For the aerosol above clouds (AAC) scenes, polarized measurements allowed the retrieval of the optical thickness (OT) and the AE of optically thin volcanic ash. We found that all the cloud parameters retrieved by passive sensors were biased due to the presence of the elevated volcanic plumes. Finally, thermal infrared measurements were used to identify the type of multilayer scene (cirrus clouds or volcanic dust above liquid clouds) and the retrieval method also provided the OT of thin cirrus layers above the clouds near Iceland.

Routine sun-photometer and micro-lidar measurements were performed in Lille, northern France, in April and May 2010 during the Eyjafjallajökull volcanic eruption. The impact of such an eruption emphasized significance of hazards for human activities and importance of observations of the volcanic aerosol particles. This paper presents the main results of a joint micro-lidar/sun-photometer analysis performed in Lille, where volcanic ash plumes were observed during at least 22 days, whenever weather conditions permitted. Aerosol properties retrieved from automatic sun-photometer measurements (AERONET) were strongly changed during the volcanic aerosol plumes transport over Lille. In most cases, the aerosol optical depth (AOD) increased, whereas Ångström exponent decreased, thus indicating coarse-mode dominance in the volume size distribution. Moreover, the non-spherical fraction retrieved by AERONET significantly increased. The real part of the complex refractive index was up to 1.55 at 440 nm during the eruption, compared to background data of about 1.46 before the eruption. Collocated lidar data revealed that several aerosol layers were present between 2 and 5 km, all originating from the Iceland region as confirmed by backward trajectories. The volcanic ash AOD was derived from lidar extinction profiles and sun-photometer AOD, and its maximum was estimated around 0.37 at 532 nm on 18 April 2010. This value was observed at an altitude of 1700 m and corresponds to an ash mass concentration (AMC) slightly higher than 1000 μg m−3 (±50%). An effective lidar ratio of ash particles of 48 sr was retrieved at 532 nm for 17 April during the early stages of the eruption, a value which agrees with several other studies carried out on this topic. Even though the accuracy of the retrievals is not as high as that obtained from reference multiwavelength lidar systems, this study demonstrates the opportunity of micro-lidar and sun-photometer joint data processing for deriving volcanic AMC. It also outlines the fact that a network of combined micro-lidars and sun photometers can be a powerful tool for routine monitoring of aerosols, especially in the case of such hazardous volcanic events.

The shortwave radiative forcing (ΔF) and the radiative forcing efficiency (ΔFeff) of natural and anthropogenic aerosols have been analyzed using estimates of radiation both at the Top (TOA) and at the Bottom Of Atmosphere (BOA) modeled based on AERONET aerosol retrievals. Six main types of atmospheric aerosols have been compared (desert mineral dust, biomass burning, urban-industrial, continental background, oceanic and free troposphere) in similar observational conditions (i.e., for solar zenith angles between 55° and 65°) in order to compare the nearly same solar geometry. The instantaneous ΔF averages obtained vary from −122 ± 37 Wm−2 (aerosol optical depth, AOD, at 0.55 μm, 0.85 ± 0.45) at the BOA for the mixture of desert mineral dust and biomass burning aerosols in West Africa and −42 ± 22 Wm−2 (AOD = 0.9 ± 0.5) at the TOA for the pure mineral dust also in this region up to −6 ± 3 Wm−2 and −4 ± 2 Wm−2 (AOD = 0.03 ± 0.02) at the BOA and the TOA, respectively, for free troposphere conditions. This last result may be taken as reference on a global scale. Furthermore, we observe that the more absorbing aerosols are overall more efficient at the BOA in contrast to at the TOA, where they backscatter less solar energy into the space. The analysis of the radiative balance at the TOA shows that, together with the amount of aerosols and their absorptive capacity, it is essential to consider the surface albedo of the region on which they are. Thus, we document that in regions with high surface reflectivity (deserts and snow conditions) atmospheric aerosols lead to a warming of the Earth-atmosphere system.

We present ground-based measurements of aerosol mass, optical properties and vertical extinction profiles acquired in M'Bour, Senegal (16.96° W; 14.39° N) from January 2006 to September 2008. This place of the world is all year long affected by the export of mineral dust as it moves westward to the north Atlantic ocean. The maximum in the dust activity is observed in summer (June–July), corresponding to a maximum in the aerosol optical thickness (above 0.5) and single scattering albedo (above 0.95). It also corresponds to a maximum in the top altitude of the transported aerosol layer (up to 6 km) and aerosol optical thickness scale height (up to 3.5 km) due to the presence of the Saharan Air Layer located between 2 and 6 km. The late summer shows an additional low level aerosol layer that increases in thickness in autumn. Severe dust storms are also systematically observed in spring (March) but with a lower vertical development and a stronger impact (factor 2 to 3) on the ground-level mass compared to summer. Sporadic events of biomass burning aerosols are observed in winter (January) and particularly in January 2006 when the biomass burning aerosol are advected between 1.5 and 3.5 km high. On average, the seasonal signal in the aerosol optical properties and vertical distribution is very similar from year to year over our 3 year monitoring.

Iron is a major component of atmospheric aerosols, influencing the light absorption ability of mineral dust, and an important micronutrient that affects oceanic biogeochemistry. The regional distribution of the iron concentration in dust is important for climate studies; however, this is difficult to obtain since it requires in-situ aerosol sampling or simulation of complex natural processes. Simultaneous studies of aerosol chemical composition and radiometric measurements of aerosol optical properties, which were performed in the Negev desert of Israel continuously for about eight years, suggest a potential for deriving a relationship between chemical composition and light absorption properties, in particular the spectral single-scattering albedo. The two main data sets of the present study were obtained by a sun/sky radiometer and a stacked filter unit sampler that collects particles in coarse and fine size fractions. Analysis of chemical and optical data showed the presence of mixed dust and pollution aerosol in the study area, although their sources appear to be different. Spectral SSA showed an evident response to increased concentrations of iron, black carbon equivalent matter, and their mixing state. A relationship that relates the spectral SSA, the percentage of iron in total particulate mass, and the pollution components was derived. Results calculated, using this relationship, were compared with measurements from dust episodes in several locations around the globe. The comparison showed reasonable agreement between the calculated and the observed iron concentrations, and supported the validity of the suggested approach for the estimation of iron concentrations in mineral dust.