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.

Global measurements of absorbing aerosol optical depth (AAOD) are scarce and mostly provided by the ground network AERONET (AErosol RObotic NETwork). In recent years, several satellite products of AAOD have been developed. This study's primary aim is to establish the usefulness of these datasets for AEROCOM (Aerosol Comparisons between Observations and Models) model evaluation with a focus on the years 2006, 2008 and 2010. The satellite products are super-observations consisting of $\mathrm{1}{}^{\circ }\times \mathrm{1}{}^{\circ }\times \mathrm{30}$ min aggregated retrievals. This study consists of two papers, the current one that deals with the assessment of satellite observations and a second paper (Schutgens et al., 2021) that deals with the evaluation of models using those satellite data. In particular, the current paper details an evaluation with AERONET observations from the sparse AERONET network as well as a global intercomparison of satellite datasets, with a focus on how minimum AOD (aerosol optical depth) thresholds and temporal averaging may improve agreement between satellite observations. All satellite datasets are shown to have reasonable skill for AAOD (three out of four datasets show correlations with AERONET in excess of 0.6) but less skill for SSA (single-scattering albedo; only one out of four datasets shows correlations with AERONET in excess of 0.6). In comparison, satellite AOD shows correlations from 0.72 to 0.88 against the same AERONET dataset. However, we show that performance vs. AERONET and inter-satellite agreements for SSA improve significantly at higher AOD. Temporal averaging also improves agreements between satellite datasets. Nevertheless multi-annual averages still show systematic differences, even at high AOD. In particular, we show that two POLDER (Polarization and Directionality of the Earth's Reflectances) products appear to have a systematic SSA difference over land of ∼0.04, independent of AOD. Identifying the cause of this bias offers the possibility of substantially improving current datasets. We also provide evidence that suggests that evaluation with AERONET observations leads to an underestimate of true biases in satellite SSA. In the second part of this study we show that, notwithstanding these biases in satellite AAOD and SSA, the datasets allow meaningful evaluation of AEROCOM models.

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.

Understanding the role atmospheric aerosols play in the Earth–atmosphere system is limited by uncertainties in the knowledge of their distribution, composition and sources. In this paper, we use the GEOS-Chem based inverse modelling framework for retrieving desert dust (DD), black carbon (BC) and organic carbon (OC) aerosol emissions simultaneously. Aerosol optical depth (AOD) and aerosol absorption optical depth (AAOD) retrieved from the multi-angular and polarimetric POLDER/PARASOL measurements generated by the GRASP algorithm (hereafter PARASOL/GRASP) have been assimilated. First, the inversion framework is validated in a series of numerical tests conducted with synthetic PARASOL-like data. These tests show that the framework allows for retrieval of the distribution and strength of aerosol emissions. The uncertainty of retrieved daily emissions in error free conditions is below 25.8 % for DD, 5.9 % for BC and 26.9 % for OC. In addition, the BC emission retrieval is sensitive to BC refractive index, which could produce an additional factor of 1.8 differences for total BC emissions. The approach is then applied to 1 year (December 2007 to November 2008) of data over the African and Arabian Peninsula region using PARASOL/GRASP spectral AOD and AAOD at six wavelengths (443, 490, 565, 670, 865 and 1020 nm). Analysis of the resulting retrieved emissions indicates 1.8 times overestimation of the prior DD online mobilization and entrainment model. For total BC and OC, the retrieved emissions show a significant increase of 209.9 %–271.8 % in comparison to the prior carbonaceous aerosol emissions. The model posterior simulation with retrieved emissions shows good agreement with both the AOD and AAOD PARASOL/GRASP products used in the inversion. The fidelity of the results is evaluated by comparison of posterior simulations with measurements from AERONET that are completely independent measurements and more temporally frequent than PARASOL observations. To further test the robustness of our posterior emissions constrained using PARASOL/GRASP, the posterior emissions are implemented in the GEOS-5/GOCART model and the consistency of simulated AOD and AAOD with other independent measurements (MODIS and OMI) demonstrates promise in applying this database for modelling studies.

In this paper, we introduce a spectral surface reflectivity climatology based on observations made by TROPOMI on board the Sentinel-5P satellite. The database contains the directionally dependent Lambertian-equivalent reflectivity (DLER) of the Earth's surface for 21 wavelength bands ranging from 328 to 2314 nm and for each calendar month. The spatial resolution of the database grid is 0.125° × 0.125°. A recently developed cloud shadow detection technique is implemented to avoid dark scenes due to cloud shadow. In the database, the anisotropy of the surface reflection is described using a third-order parameterisation of the viewing angle dependence. The viewing angle dependence of the DLER is analysed globally and for a selection of surface type regions. The dependence is found to agree with the viewing angle dependence found in the GOME-2 surface DLER database. Differences exist, related to the actual solar position. On average, the viewing angle dependence in TROPOMI DLER is weaker than for GOME-2 DLER, but still important. Validation of the new database was first performed by comparison of the non-directional TROPOMI surface LER with heritage LER databases based on GOME-1, OMI, SCIAMACHY, and GOME-2 data. Agreement was found within 0.002–0.02 in the UV-VIS (below 500 nm), up to 0.003 in the NIR (670–772 nm), and below 0.001 in the short-wave infrared (SWIR) (2314 nm). These performance numbers are dominated by the performance over ocean, but they are in most cases also representative for land surfaces. For the validation of the directional TROPOMI surface DLER, we made use of comparison with the MODIS surface bi-directional reflectance distribution function (BRDF) for a selection of surface type regions. In all cases the DLER performed significantly better than the traditional LER, and we found good agreement with the MODIS surface BRDF. The TROPOMI surface DLER database is a clear improvement on previous surface albedo databases and can be used as input not only for satellite retrievals from TROPOMI observations, but also for retrievals from observations from other polar-orbiting satellite instruments provided that their equator crossing time is close to that of TROPOMI. The algorithm that is introduced in this paper can be used for the retrieval of surface reflectivity climatologies from other polar satellite missions as well, including Ocean and Land Colour Instrument (OLCI) on the Sentinel-3 satellites, Sentinel-5, and Multi-viewing Multi-channel Multi-polarisation imager (3MI) on the MetOp-SG-A1 satellite to be launched in 2025, as well as the future CO2M mission.

From a passive satellite remote sensing point of view, the richest set of information on aerosol properties can be obtained from instruments that measure both intensity and polarization of backscattered sunlight at multiple wavelengths and multiple viewing angles for one ground pixel. However, it is challenging to exploit this information at a global scale because complex algorithms are needed with many fit parameters (aerosol and land/ocean reflection), based on online radiative transfer models. So far, two such algorithms have demonstrated this capability at a global scale: the Generalized Retrieval of Atmosphere and Surface Properties (GRASP) algorithm and the Remote sensing of Trace gas and Aerosol Products (RemoTAP) algorithm. In this paper, we present a detailed comparison of the most recent versions of RemoTAP and GRASP. We evaluate both algorithms for synthetic observations, for real PARASOL (Polarization and Anisotropy of Reflectances for Atmospheric Science coupled with Observations from a Lidar) observations against AERONET (Aerosol Robotic Network) for common pixels, and for global PARASOL retrievals for the year 2008. For the aerosol optical depth (AOD) over land, both algorithms show a root mean square error (RMSE) of 0.10 (at 550 nm). For single scattering albedo (SSA), both algorithms show a good performance in terms of RMSE (0.04), but RemoTAP has a smaller bias (0.002) compared to GRASP (0.021). For the Ångström exponent (AE), GRASP has a smaller RMSE (0.367) than RemoTAP (0.387), mainly caused by a small overestimate of AE at low values (large particles). Over ocean both algorithms perform very well. For AOD, RemoTAP has an RMSE of 0.057 and GRASP an even smaller RMSE of 0.047. For AE, the RMSEs of RemoTAP and GRASP are 0.285 and 0.224, respectively. Based on the AERONET comparison, we conclude that both algorithms show very similar overall performance, where both algorithms have stronger and weaker points. For the global data products, we find a root mean square difference (RMSD) between RemoTAP and GRASP AOD of 0.12 and 0.038 over land and ocean, respectively. The largest differences occur over the biomass burning region in equatorial Africa. The global mean values are virtually unbiased with respect to each other. For AE the RMSD between RemoTAP and GRASP is 0.33 over land and 0.23 over ocean. For SSA, we find much better agreement over land (bias = −0.01, RMSD = 0.043 for retrievals with AOD > 0.2) than over ocean (bias = 0.053, RMSD = 0.074). As expected, the differences increase towards low AOD, over both land and ocean. We also compared the GRASP and RemoTAP AOD and AE products against MODIS. For AOD over land, the agreement of either GRASP or RemoTAP with MODIS is worse than the agreement between the two PARASOL algorithms themselves. Over ocean, the agreement is very similar among the three products for AOD. For AE, the agreement between GRASP and RemoTAP is much better than the agreement of both products with MODIS. The agreement of the latest product versions with each other and with AERONET improved significantly compared to the previous version of the global products of GRASP and RemoTAP. The results demonstrate that the dedicated effort in algorithm development for multi-angle polarimetric (MAP) aerosol retrievals still leads to substantial improvement of the resulting aerosol products, and this is still an ongoing process.