Comprehensive tool for calculation of radiative fluxes: illustration of shortwave aerosol radiative effect sensitivities to the details in aerosol and underlying surface characteristics

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

Information content and aerosol property retrieval potential for different types of in situ polar nephelometer data

Polar nephelometers are in situ instruments used to measure the angular distribution of light scattered by aerosol particles. These types of measurements contain substantial information about the properties of the aerosol being probed (e.g. concentrations, sizes, refractive indices, shape parameters), which can be retrieved through inversion algorithms. The aerosol property retrieval potential (i.e. information content) of a given set of measurements depends on the spectral, polarimetric, and angular characteristics of the polar nephelometer that was used to acquire the measurements. To explore this issue quantitatively, we applied Bayesian information content analysis and calculated the metric degrees of freedom for signal (DOFS) for a range of simulated polar nephelometer instrument configurations, aerosol models and test cases, and assumed levels of prior knowledge about the variances of specific aerosol properties. Assuming a low level of prior knowledge consistent with an unconstrained ambient/field measurement setting, we demonstrate that even very basic polar nephelometers (single wavelength, no polarization capability) will provide informative measurements with a very high retrieval potential for the size distribution and refractive index state parameters describing simple unimodal, spherical test aerosols. As expected, assuming a higher level of prior knowledge consistent with well-constrained laboratory applications leads to a reduction in potential for information gain via performing the polarimetric measurement. Nevertheless, we show that in this situation polar nephelometers can still provide informative measurements: e.g. it can be possible to retrieve the imaginary part of the refractive index with high accuracy if the laboratory setting makes it possible to keep the probed aerosol sample simple. The analysis based on a high level of prior knowledge also allows us to better assess the impact of different polar nephelometer instrument design features in a consistent manner for retrieved aerosol parameters. The results indicate that the addition of multi-wavelength and/or polarimetric measurement capabilities always leads to an increase in information content, although in some cases the increase is negligible, e.g. when adding a fourth, near-IR measurement wavelength for the retrieval of unimodal size distribution parameters or if the added polarization component has high measurement uncertainty. By considering a more complex bimodal, non-spherical-aerosol model, we demonstrate that performing more comprehensive spectral and/or polarimetric measurements leads to very large benefits in terms of the achieved information content. We also investigated the impact of angular truncation (i.e. the loss of measurement information at certain scattering angles) on information content. Truncation at extreme angles (i.e. in the near-forward or near-backward directions) results in substantial decreases in information content for coarse-aerosol test cases. However for fine-aerosol test cases, the sensitivity of DOFS to extreme-angle truncation is noticeably smaller and can be further reduced by performing more comprehensive measurements. Side angle truncation has very little effect on information content for both the fine and coarse test cases. Furthermore, we demonstrate that increasing the number of angular measurements generally increases the information content. However, above a certain number of angular measurements (∼20–40) the observed increases in DOFS plateau out. Finally, we demonstrate that the specific placement of angular measurements within a nephelometer can have a large impact on information content. As a proof of concept, we show that a reductive greedy algorithm based on the DOFS metric can be used to find optimal angular configurations for given target aerosols and applications.</p

Information content and aerosol property retrieval potential for different types of in situ polar nephelometer data

Polar nephelometers are in situ instruments used to measure the angular distribution of light scattered by aerosol particles. These type of measurements contain substantial information about the properties of the aerosol being probed (e.g. concentrations, sizes, refractive indices, shape parameters), which can be retrieved through inversion algorithms. The aerosol property retrieval potential (i.e., information content) of a given set of measurements depends on the spectral, polarimetric and angular characteristics of the polar nephelometer that was used to acquire it. To explore this issue quantitatively, we applied Bayesian information content analysis and calculated the metric Degrees of Freedom for Signal (DOFS) for a range of simulated polar nephelometer instrument configurations, aerosol models and test cases, and assumed levels of prior knowledge about the variances of specific aerosol properties. Assuming a low level of prior knowledge consistent with an unconstrained ambient/field measurement setting, we demonstrate that even very basic polar nephelometers (single wavelength, no polarization capability) will provide informative measurements with very high retrieval potential for the size distribution and refractive index state parameters describing simple unimodal, spherical test aerosols. As expected, assuming a higher level of prior knowledge consistent with well constrained laboratory applications leads to a reduction in potential for information gain via performing the polarimetric measurement. This analysis allows us to better assess the impact of different polar nephelometer instrument design features in a consistent manner for retrieved aerosol parameters. The results indicate that the addition of multi-wavelength and/or polarimetric measurement capabilities always leads to an increase in information content, although in some cases the increase is negligible: e.g. when adding a fourth, near-IR measurement wavelength for the retrieval of unimodal size distribution parameters, or if the added polarization component has high measurement uncertainty. By considering a more complex bimodal, non-spherical aerosol model, we demonstrate that performing the more comprehensive spectral and/or polarimetric measurements leads to very large benefits in terms of the achieved information content. We also investigated the impact of angular truncation (i.e., the loss of measurement information at certain scattering angles) on information content. Truncation at extreme angles (i.e., in the near-forward or &ndash;backward directions) results in substantial decreases in information content for coarse aerosol test cases. However for fine aerosol test cases, the sensitivity of DOFS to extreme angle truncation is noticeably smaller and can be further reduced by performing more comprehensive measurements. Side-angle truncation has very little effect on information content for both the fine and coarse test cases. Furthermore, we demonstrate that increasing the number of angular measurements generally increases the information content. However, above a certain number of angular measurements (~20&ndash;40) the observed increases in DOFS plateau out. Finally, we demonstrate that the specific placement of angular measurements within a nephelometer can have a large impact on information content. As a proof-of-concept, we show that a reductive greedy algorithm based on the DOFS metric can be used to find optimal angular configurations for given target aerosols and applications.</p

Properties of aerosol and surface derived from OLCI/Sentinel-3A using GRASP approach: Retrieval development and preliminary validation

The Ocean and Land Color Instrument (OLCI) onboard the Copernicus Sentinel-3A satellite is a medium-resolution and multi-spectral push-broom imager acquiring radiance in 21 spectral bands covering from the visible to the far near-infrared. These measurements are primary dedicated to land & ocean color applications, but actually include also reliable information for atmospheric aerosol and surface brightness characterization. In the framework of the EUMETSAT funded study to support the Copernicus Program, we describe the retrieval of aerosol and surface properties from OLCI single-viewing multi-spectral Top-Of-Atmosphere (TOA) radiances based on the Generalized Retrieval of Atmosphere and Surface Properties (GRASP) algorithm. The high potential of the OLCI/GRASP configuration stems from the attempt to retrieve both aerosol load and surface reflectance simultaneously using a globally consistent high-level approach. For example, both over land and ocean surfaces OLCI/GRASP uses 9 spectral channels (albeit with different weights), strictly the same prescribed aerosol models and globally the same a priori constraints (though with some differences for observations over land and ocean). Due to the lack of angular multi-viewing information, the directional properties of underlying surface are strongly constrained in the retrieval: over ocean the Fresnel reflection together with foam/whitecap albedo are exclusively computed using a priori wind speed; over land, the Bidirectional Reflectance Distribution Function (BRDF) is slightly adjusted from a priori values of climatological Ross-Li volumetric and geometric terms. Meanwhile, the isotropic reflectance is retrieved globally under mild spectral smoothness constraints. It should be noticed that OLCI/GRASP configuration employs innovative multi-pixel concept (Dubovik et al., 2011) that enhance retrieval by simultaneously inverting large group of pixels. The concept allows for benefiting from knowledge about natural variability of the retrieved parameters. The obtained OLCI/GRASP products were validated with the Aerosol Robotic Network (AERONET) and Maritime Aerosol Network (MAN) and intercompared with the Moderate Resolution Imaging Spectroradiometer (MODIS) aerosol and surface products. The overall performance is quite comparable to the community-referenced MODIS. Over ocean the OLCI/GRASP results are encouraging with 67% of the AOD (550 nm) satisfying the Global Climate Observing System (GCOS) requirement using AERONET coastal sites and 74% using MAN deep ocean measurements, and an AOD (550 nm) bias 0.01 with AERONET and nearly zero bias with MAN. Over land, 48% of OLCI/GRASP AOD (550 nm) satisfy the GCOS requirement and a bias within ±0.01 for total and AOD < 0.2. Key challenges are identified and discussed: adequate screening of cloud contaminations, retrieval of aerosol over bright surfaces and in the regions containing complex mixtures of aerosol

Retrievals of Aerosol Optical and Microphysical Properties from Imaging Polar Nephelometer Scattering Measurements

A method for the retrieval of aerosol optical and microphysical properties from in situ light-scattering measurements is presented and the results are compared with existing measurement techniques. The Generalized Retrieval of Aerosol and Surface Properties (GRASP) is applied to airborne and laboratory measurements made by a novel polar nephelometer. This instrument, the Polarized Imaging Nephelometer (PI-Neph), is capable of making high-accuracy field measurements of phase function and degree of linear polarization, at three visible wavelengths, over a wide angular range of 3 to 177. The resulting retrieval produces particle size distributions (PSDs) that agree, within experimental error, with measurements made by commercial optical particle counters (OPCs). Additionally, the retrieved real part of the refractive index is generally found to be within the predicted error of 0.02 from the expected values for three species of humidified salt particles, with a refractive index that is well established. The airborne measurements used in this work were made aboard the NASA DC-8 aircraft during the Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) field campaign, and the inversion of this data represents the first aerosol retrievals of airborne polar nephelometer data. The results provide confidence in the real refractive index product, as well as in the retrieval's ability to accurately determine PSD, without assumptions about refractive index that are required by the majority of OPCs

Multi-angular polarimetric remote sensing to pinpoint global aerosol absorption and direct radiative forcing

Quantitative estimations of atmospheric aerosol absorption are rather uncertain due to the lack of reliable information about the global distribution. Because the information about aerosol properties is commonly provided by single-viewing photometric satellite sensors that are not sensitive to aerosol absorption. Consequently, the uncertainty in aerosol radiative forcing remains one of the largest in the Assessment Reports of the Intergovernmental Panel on Climate Change (IPCC AR5 and AR6). Here, we use multi-angular polarimeters (MAP) to provide constraints on emission of absorbing aerosol species and estimate global aerosol absorption optical depth (AAOD) and its climate effect. Our estimate of modern-era mid-visible AAOD is 0.0070 that is higher than IPCC by a factor of 1.3-1.8. The black carbon instantaneous direct radiative forcing (BC DRF) is +0.33&thinsp;W/m2 [+0.17, +0.54]. The MAP constraint narrows the 95% confidence interval of BC DRF by a factor of 2 and boosts confidence in its spatial distribution. &nbsp;</p

Estimates of remote sensing retrieval errors by the GRASP algorithm: application to ground-based observations, concept and validation

Understanding the uncertainties in the retrieval of aerosol and surface properties is very important for an adequate characterization of the processes that occur in the atmosphere. However, the reliable characterization of the error budget of the retrieval products is a very challenging aspect that currently remains not fully resolved in most remote sensing approaches. The level of uncertainties for the majority of the remote sensing products relies mostly on post-processing validations and intercomparisons with other data, while the dynamic errors are rarely provided. Therefore, implementations of fundamental approaches for generating dynamic retrieval errors and the evaluation of their practical efficiency remains of high importance. This study describes and analyses the dynamic estimates of uncertainties in aerosol-retrieved properties by the GRASP (Generalized Retrieval of Atmosphere and Surface Properties) algorithm. The GRASP inversion algorithm, described by Dubovik et al. (2011, 2014, 2021), is designed based on the concept of statistical optimization and provides dynamic error estimates for all retrieved aerosol and surface properties. The approach takes into account the effect of both random and systematic uncertainties propagations. The algorithm provides error estimates both for directly retrieved parameters included in the retrieval state vector and for the characteristics derived from these parameters. For example, in the case of the aerosol properties, GRASP directly retrieves the size distribution and the refractive index that are used afterwards to provide phase function, scattering, extinction, single scattering albedo, etc. Moreover, the GRASP algorithm provides full covariance matrices, i.e. not only variances of the retrieval errors but also correlations coefficients of these errors. The analysis of the correlation matrix structure can be very useful for identifying less than obvious retrieval tendencies. This appears to be a useful approach for optimizing observation schemes and retrieval set-ups. In this study, we analyse the efficiency of the GRASP error estimation approach for applications to ground-based observations by a sun/sky photometer and lidar. Specifically, diverse aspects of the error generations and their evaluations are discussed and illustrated. The studies rely on a series of comprehensive sensitivity tests when simulated sun/sky photometer measurements and lidar data are perturbed by random and systematic errors and inverted. Then, the results of the retrievals and their error estimations are analysed and evaluated. The tests are conducted for different observations of diverse aerosol types, including biomass burning, urban, dust and their mixtures. The study considers observations of AErosol RObotic NETwork (AERONET) sun/sky photometer measurements at 440, 675, 870 and 1020 nm and multiwavelength elastic lidar measurements at 355, 532 and 1064 nm. The sun/sky photometer data are inverted alone or together with lidar data. The analysis shows overall successful retrievals and error estimations for different aerosol characteristics, including aerosol size distribution, complex refractive index, single scattering albedo, lidar ratios, aerosol vertical profiles, etc. Also, the main observed tendencies in the error dynamic agree with known retrieval experience. For example, the main accuracy limitations for retrievals of all aerosol types relate to the situations with low optical depth. Also, in situations with multicomponent aerosol mixtures, the reliable characterization of each component is possible only in limited situations, for example, from radiometric data obtained for low solar zenith angle observations or from a combination of radiometric and lidar data. At the same time, the total optical properties of aerosol mixtures are always retrieved satisfactorily. In addition, the study includes an analysis of the detailed structure of the correlation matrices for the retrieval errors in mono- and multicomponent aerosols. The conducted analysis of error correlation appears to be a useful approach for optimizing observation schemes and retrieval set-ups. The application of the approach to real data is provided.</p

Microscopic observations of core-shell particle structure and implications for atmospheric aerosol remote sensing

International audienceTropospheric aerosols play an important role in atmospheric chemistry, Earth’s radiative budget, and climate.After their generation, aerosols can suffer ageing processes and alter their physicochemical properties. Anaccurate accounting for these processes requires observations of the aerosol properties on different temporaland spatial scales. The current work is dedicated to: (i) study of physicochemical properties and mixing state ofindividual particles by means of analytical scanning and transmission electron microscopy for aerosolscollected during episodes of elevated aerosol loading; (ii) analysis of the effect of microphysical properties onoptical characteristics as measured and retrieved by remote sensing; and (iii) investigation of possibleparameterization of aerosol composition and core-shell structure in remote sensing algorithms. The workpresents observations conducted in northern France and western Africa (Senegal) as part of Labex CaPPAproject and SHADOW field campaigns. It includes simultaneous analyses of collected individual particles’composition and structure, remote sensing and in situ observations of urban/industrial, Saharan dust andbiomass burning particles near the surface and at different altitudes. A series of numerical simulations devotedto an analysis of the sensitivity of remote sensing observations to aerosol mixing state is conducted. Insights ona possible parameterization of aerosol core-shell structure in retrieval algorithms are finally presented

Utilization of AERONET polarimetric measurements for improving retrieval of aerosol microphysics: GSFC, Beijing and Dakar data analysis

International audienceThe study presents the efforts on including the polarimetric data to the routine inversion of the radiometric ground-based measurements for characterization of the atmospheric aerosols and analysis of the obtained advantages in retrieval results. First, to operationally process the large amount of polarimetric data the data preparation tool was developed. The AERONET inversion code adapted for inversion of both intensity and polarization measurements was used for processing. Second, in order to estimate the effect from utilization of polarimetric information on aerosol retrieval results, both synthetic data and the real measurements were processed using developed routine and analyzed. The sensitivity study has been carried out using simulated data based on three main aerosol models: desert dust, urban industrial and urban clean aerosols. The test investigated the effects of utilization of polarization data in the presence of random noise, bias in measurements of optical thickness and angular pointing shift. The results demonstrate the advantage of polarization data utilization in the cases of aerosols with pronounced concentration of fine particles. Further, the extended set of AERONET observations was processed. The data for three sites have been used: GSFC, USA (clean urban aerosol dominated by fine particles), Beijing, China (polluted industrial aerosol characterized by pronounced mixture of both fine and coarse modes) and Dakar, Senegal (desert dust dominated by coarse particles). The results revealed considerable advantage of polarimetric data applying for characterizing fine mode dominated aerosols including industrial pollution (Beijing). The use of polarization corrects particle size distribution by decreasing overestimated fine mode and increasing the coarse mode. It also increases underestimated real part of the refractive index and improves the retrieval of the fraction of spherical particles due to high sensitivity of polarization to particle shape. Overall, the study demonstrates a substantial value of polarimetric data for improving aerosol characterization