First close insight into global daily gapless 1 km PM2.5 pollution, variability, and health impact.

Here we retrieve global daily 1 km gapless PM2.5 concentrations via machine learning and big data, revealing its spatiotemporal variability at an exceptionally detailed level everywhere every day from 2017 to 2022, valuable for air quality monitoring, climate change, and public health studies. We find that 96%, 82%, and 53% of Earth's populated areas are exposed to unhealthy air for at least one day, one week, and one month in 2022, respectively. Strong disparities in exposure risks and duration are exhibited between developed and developing countries, urban and rural areas, and different parts of cities. Wave-like dramatic changes in air quality are clearly seen around the world before, during, and after the COVID-19 lockdowns, as is the mortality burden linked to fluctuating air pollution events. Encouragingly, only approximately one-third of all countries return to pre-pandemic pollution levels. Many nature-induced air pollution episodes are also revealed, such as biomass burning.

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 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.

Extensive characterization of aerosol optical properties and chemical component concentrations: Application of the GRASP/Component approach to long-term AERONET measurements.

A recently developed GRASP/Component approach (GRASP: Generalized Retrieval of Atmosphere and Surface Properties) was applied to AERONET (Aeronet Robotic Network) sun photometer measurements in this study. Unlike traditional aerosol component retrieval, this approach allows the inference of some information about aerosol composition directly from measured radiance, rather than indirectly through the inversion of optical parameters, and has been integrated into the GRASP algorithm. The newly developed GRASP/Component approach was applied to 13 AERONET sites for different aerosol types under the assumption of aerosol internal mixing rules to analyze the characteristics of aerosol components and their distribution patterns. The results indicate that the retrievals can characterize well the spatial and temporal variability of the component concentration for different aerosol types. A reasonable agreement between GRASP BC retrievals and MERRA-2 BC products is found for all different aerosol types. In addition, the relationships between aerosol component content and aerosol optical parameters such as aerosol optical depth (AOD), fine-mode fraction (FMF), absorption Ångström exponent (AAE), scattering Ångström exponent (SAE), and single scattering albedo (SSA) are also analyzed for indirect verifying the reliability of the component retrieval. It was demonstrated the GRASP/Component optical retrievals are in good agreement with AERONET standard products [e.g., correlation coefficient (R) of 0.93-1.0 for AOD, fine-mode AOD (AODF), coarse-mode AOD (AODC) and Ångström exponent (AE); R = ~ 0.8 for absorption AOD (AAOD) and SSA; RMSE (root mean square error) < 0.03 for AOD, AODF, AODC, AAOD and SSA]. Thus, it is demonstrated the GRASP/Component approach can provide aerosol optical products with comparable accuracy as the AERONET standard products from the ground-based sun photometer measurements as well as some additional important inside on aerosol composition.

Climate models generally underrepresent the warming by Central Africa biomass-burning aerosols over the Southeast Atlantic.

The radiative budget, cloud properties, and precipitation over tropical Africa are influenced by solar absorption by biomass-burning aerosols (BBA) from Central Africa. Recent field campaigns, reinforced by new remote-sensing and aerosol climatology datasets, have highlighted the absorbing nature of the elevated BBA layers over the South-East Atlantic (SEA), indicating that the absorption could be stronger than previously thought. We show that most of the latest generation of general circulation models (GCMs) from the sixth phase of the Coupled Model Intercomparison Project 6 (CMIP6) underestimates the absorption of BBA over the SEA. This underlines why many (~75%) CMIP6 models do not fully capture the intense positive (warming) direct radiative forcing at the top of the atmosphere observed over this region. In addition, underestimating the magnitude of the BBA-induced solar heating could lead to misrepresentations of the low-level cloud responses and fast precipitation feedbacks that are induced by BBA in tropical regions.

Effects of the shape distribution of aerosol particles on their volumetric scattering properties and the radiative transfer through the atmosphere that includes polarization.

In this paper, we investigate the effects of shape distribution of aerosol particles on the volumetric scattering properties, as well as the radiance and polarization distributions of skylight, by numerical simulations. The results demonstrate that the shape distribution indeed exerts a significant influence on the skylight degree of linear polarization. The skylight polarization calculated assuming the microscope-measured shape distributions is distinct from that using the inversion-based shape distributions. The significant effects will influence the retrieval of the sphericity of aerosols based on the sun-sky radiometer measurements. Our results suggest that using representative shape distributions obtained by direct microscopic observations of aerosol samples captured in the natural atmosphere has a high potential to improve the retrieval of the aerosol shape parameter.

Atmospheric Correction of Satellite Ocean-Color Imagery During the PACE Era.

The Plankton, Aerosol, Cloud, ocean Ecosystem (PACE) mission will carry into space the Ocean Color Instrument (OCI), a spectrometer measuring at 5nm spectral resolution in the ultraviolet (UV) to near infrared (NIR) with additional spectral bands in the shortwave infrared (SWIR), and two multi-angle polarimeters that will overlap the OCI spectral range and spatial coverage, i. e., the Spectrometer for Planetary Exploration (SPEXone) and the Hyper-Angular Rainbow Polarimeter (HARP2). These instruments, especially when used in synergy, have great potential for improving estimates of water reflectance in the post Earth Observing System (EOS) era. Extending the top-of-atmosphere (TOA) observations to the UV, where aerosol absorption is effective, adding spectral bands in the SWIR, where even the most turbid waters are black and sensitivity to the aerosol coarse mode is higher than at shorter wavelengths, and measuring in the oxygen A-band to estimate aerosol altitude will enable greater accuracy in atmospheric correction for ocean color science. The multi-angular and polarized measurements, sensitive to aerosol properties (e.g., size distribution, index of refraction), can further help to identify or constrain the aerosol model, or to retrieve directly water reflectance. Algorithms that exploit the new capabilities are presented, and their ability to improve accuracy is discussed. They embrace a modern, adapted heritage two-step algorithm and alternative schemes (deterministic, statistical) that aim at inverting the TOA signal in a single step. These schemes, by the nature of their construction, their robustness, their generalization properties, and their ability to associate uncertainties, are expected to become the new standard in the future. A strategy for atmospheric correction is presented that ensures continuity and consistency with past and present ocean-color missions while enabling full exploitation of the new dimensions and possibilities. Despite the major improvements anticipated with the PACE instruments, gaps/issues remain to be filled/tackled. They include dealing properly with whitecaps, taking into account Earth-curvature effects, correcting for adjacency effects, accounting for the coupling between scattering and absorption, modeling accurately water reflectance, and acquiring a sufficiently representative dataset of water reflectance in the UV to SWIR. Dedicated efforts, experimental and theoretical, are in order to gather the necessary information and rectify inadequacies. Ideas and solutions are put forward to address the unresolved issues. Thanks to its design and characteristics, the PACE mission will mark the beginning of a new era of unprecedented accuracy in ocean-color radiometry from space.

Studying aerosol light scattering based on aspect ratio distribution observed by fluorescence microscope.

Particle shape is crucial to the properties of light scattered by atmospheric aerosol particles. A method of fluorescence microscopy direct observation was introduced to determine the aspect ratio distribution of aerosol particles. The result is comparable with that of the electron microscopic analysis. The measured aspect ratio distribution has been successfully applied in modeling light scattering and further in simulation of polarization measurements of the sun/sky radiometer. These efforts are expected to improve shape retrieval from skylight polarization by using directly measured aspect ratio distribution.

Reducing Multi-sensor Monthly Mean Aerosol Optical Depth Uncertainty Part II: Optimal Locations for Potential Ground Observation Deployments.

Surface remote sensing of aerosol properties provides "ground truth" for satellite and model validation, and is an important component of aerosol observation system. Due to the different characteristics of background aerosol variability, information obtained at different locations usually have different spatial representativeness, implying that the location should be carefully chosen so that its measurement could be extended to a greater area. In this study, we present an objective observation array design technique that automatically determines the optimal locations with the highest spatial representativeness based on the Ensemble Kalman Filter (EnKF) theory. The ensemble is constructed using aerosol optical depth (AOD) products from five satellite sensors. The optimal locations are solved sequentially by minimizing the total analysis error variance, which means that observations at these locations will reduce the background error variance to the largest extent. The location determined by the algorithm is further verified to have larger spatial representativeness than some other arbitrary location. In addition to the existing active AERONET sites, the 40 selected optimal locations are mostly concentrated on regions with both high AOD inhomogeneity and its spatial representativeness, namely the Sahel, South Africa, East Asia and North Pacific Islands. These places should be the focuses of establishing future AERONET sites in order to further reduce the uncertainty in the monthly mean AOD. Observations at these locations contribute to approximately 50% of the total background uncertainty reduction.

Advanced characterisation of aerosol size properties from measurements of spectral optical depth using the GRASP algorithm.

This study evaluates the potential of using aerosol optical depth (τ a) measurements to characterise the microphysical and optical properties of atmospheric aerosols. With this aim, we used the recently developed GRASP (Generalized Retrieval of Aerosol and Surface Properties) code for numerical testing of six different aerosol models with different aerosol loads. The direct numerical simulations (self-consistency tests) indicate that the GRASP-AOD retrieval provides modal aerosol optical depths (fine and coarse) to within 0.01 of the input values. The retrieval of the fine-mode radius, width and volume concentration are stable and precise if the real part of the refractive index is known. The coarse-mode properties are less accurate, but they are significantly improved when additional a priori information is available. The tests with random simulated errors show that the uncertainty in the bimodal log-normal size distribution parameters increases as the aerosol load decreases. Similarly, the reduction in the spectral range diminishes the stability of the retrieved parameters. In addition to these numerical studies, we used optical depth observations at eight AERONET locations to validate our results with the standard AERONET inversion products. We found that bimodal log-normal size distributions serve as useful input assumptions, especially when the measurements have inadequate spectral coverage and/or limited accuracy, such as moon photometry. Comparisons of the mode median radii between GRASP-AOD and AERONET indicate average differences of 0.013 µm for the fine mode and typical values of 0.2-0.3 µm for the coarse mode. The dominant mode (i.e. fine or coarse) indicates a 10 % difference in mode radii between the GRASP-AOD and AERONET inversions, and the average of the difference in volume concentration is around 17 % for both modes. The retrieved values of the fine-mode τ a(500) using GRASP-AOD are generally between those values obtained by the standard AERONET inversion and the values obtained by the AERONET spectral deconvolution algorithm (SDA), with differences typically lower than 0.02 between GRASP-AOD and both algorithms. Finally, we present some examples of application of GRASP-AOD inversion using moon photometry and the airborne PLASMA sun photometer during the ChArMEx summer 2013 campaign in the western Mediterranean.

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.

Reducing multisensor satellite monthly mean aerosol optical depth uncertainty: 1. Objective assessment of current AERONET locations.

Various space-based sensors have been designed and corresponding algorithms developed to retrieve aerosol optical depth (AOD), the very basic aerosol optical property, yet considerable disagreement still exists across these different satellite data sets. Surface-based observations aim to provide ground truth for validating satellite data; hence, their deployment locations should preferably contain as much spatial information as possible, i.e., high spatial representativeness. Using a novel Ensemble Kalman Filter (EnKF)-based approach, we objectively evaluate the spatial representativeness of current Aerosol Robotic Network (AERONET) sites. Multisensor monthly mean AOD data sets from Moderate Resolution Imaging Spectroradiometer, Multiangle Imaging Spectroradiometer, Sea-viewing Wide Field-of-view Sensor, Ozone Monitoring Instrument, and Polarization and Anisotropy of Reflectances for Atmospheric Sciences coupled with Observations from a Lidar are combined into a 605-member ensemble, and AERONET data are considered as the observations to be assimilated into this ensemble using the EnKF. The assessment is made by comparing the analysis error variance (that has been constrained by ground-based measurements), with the background error variance (based on satellite data alone). Results show that the total uncertainty is reduced by ~27% on average and could reach above 50% over certain places. The uncertainty reduction pattern also has distinct seasonal patterns, corresponding to the spatial distribution of seasonally varying aerosol types, such as dust in the spring for Northern Hemisphere and biomass burning in the fall for Southern Hemisphere. Dust and biomass burning sites have the highest spatial representativeness, rural and oceanic sites can also represent moderate spatial information, whereas the representativeness of urban sites is relatively localized. A spatial score ranging from 1 to 3 is assigned to each AERONET site based on the uncertainty reduction, indicating its representativeness level.

Vertical profiles of pure dust and mixed smoke-dust plumes inferred from inversion of multiwavelength Raman/polarization lidar data and comparison to AERONET retrievals and in situ observations.

We present for the first time vertical profiles of microphysical properties of pure mineral dust (largely unaffected by any other aerosol types) on the basis of the inversion of optical data collected with multiwavelength polarization Raman lidar. The data were taken during the Saharan Mineral Dust Experiment (SAMUM) in Morocco in 2006. We also investigated two cases of mixed dust-smoke plumes on the basis of data collected during the second SAMUM field campaign that took place in the Republic of Cape Verde in 2008. Following the experience of the Aerosol Robotic Network (AERONET), the dust is modeled as a mixture of spherical particles and randomly oriented spheroids. The retrieval is performed from the full set of lidar input data (three backscatter coefficients, two extinction coefficients, and one depolarization ratio) and from a reduced set of data in which we exclude the depolarization ratio. We find differences of the microphysical properties depending on what kind of optical data combination we use. For the case of pure mineral dust, the results from these two sets of optical data are consistent and confirm the validity of the spheroid particle model for data inversion. Our results indicate that in the case of pure mineral dust we do not need depolarization information in the inversion. For the mixture of dust and biomass burning, there seem to be more limitations in the retrieval accuracy of the various data products. The evaluation of the quality of our data products is done by comparing our lidar-derived data products (vertically resolved) to results from AERONET Sun photometer observations (column-averaged) carried out at the lidar field site. Our results for dust effective radius show agreement with the AERONET observations within the retrieval uncertainties. Regarding the complex refractive index a comparison is difficult, as AERONET provides this parameter as wavelength-dependent quantity. In contrast, our inversion algorithm provides this parameter as a wavelength-independent quantity. We also show some comparison to results from airborne in situobservation. A detailed comparison to in situ results will be left for a future contribution.

Global atmospheric black carbon inferred from AERONET.

AERONET, a network of well calibrated sunphotometers, provides data on aerosol optical depth and absorption optical depth at >250 sites around the world. The spectral range of AERONET allows discrimination between constituents that absorb most strongly in the UV region, such as soil dust and organic carbon, and the more ubiquitously absorbing black carbon (BC). AERONET locations, primarily continental, are not representative of the global mean, but they can be used to calibrate global aerosol climatologies produced by tracer transport models. We find that the amount of BC in current climatologies must be increased by a factor of 2-4 to yield best agreement with AERONET, in the approximation in which BC is externally mixed with other aerosols. The inferred climate forcing by BC, regardless of whether it is internally or externally mixed, is approximately 1 W/m2, most of which is probably anthropogenic. This positive forcing (warming) by BC must substantially counterbalance cooling by anthropogenic reflective aerosols. Thus, especially if reflective aerosols such as sulfates are reduced, it is important to reduce BC to minimize global warming.