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While the use and data assimilation (DA) of operational Moderate Resolution Imaging Spectroradiometer (MODIS) aerosol data is commonplace, MODIS is scheduled to sunset in the next year. For data continuity, focus has turned to the development of next-generation aerosol products and sensors such as those associated with the Visible Infrared Imaging Radiometer Suite (VIIRS) on Suomi NPOESS Preparation Project (S-NPP) and NOAA-20. Like MODIS algorithms, products from these sensors require their own set of extensive error characterization and correction exercises. This is particularly true in the context of monitoring significant aerosol events that tax an algorithm's ability to separate cloud from aerosol and account for multiple scattering related errors exacerbated by uncertainties in aerosol optical properties. To investigate the performance of polar-orbiting satellite algorithms to monitor and characterize significant events, a level 3 (L3) product has been developed using a consistent aggregation methodology for 4 years of observations (2016–2019) that is referred to as the SSEC/NRL L3 product. Included in this product are the AErosol RObotic NETwork (AERONET), MODIS Dark Target, Deep Blue, and Multi-Angle Implementation of Atmospheric Correction (MAIAC) algorithms. These MODIS “baseline algorithms” are compared to NASA's recently released NASA Deep Blue algorithm for use with VIIRS. Using this new dataset, the relative performance of the algorithms for both land and ocean were investigated with a focus on the relative skill of detecting severe events and accuracy of the retrievals using AERONET. Maps of higher-percentile aerosol optical depth (AOD) regions of the world by product identified those with the highest measured AODs and determined what is high by local standards. While patterns in AOD match across products and median to moderate AOD values match well, there are regionally correlated biases between products based on sampling, algorithm differences, and AOD range – in particular for higher AOD events. Most notable are differences in boreal biomass burning and Saharan dust. Significant percentile biases must be accounted for when data are used in trend studies, data assimilation, or inverse modeling. These biases vary by aerosol regime and are likely due to retrieval assumptions in lower boundary conditions and aerosol optical models.

Atmospheric aerosols and their impact on cloud properties remain the largest uncertainty in the human forcing of the climate system. By increasing the concentration of cloud droplets (Nd), aerosols reduce droplet size and increase the reflectivity of clouds (a negative radiative forcing). Central to this climate impact is the susceptibility of cloud droplet number to aerosol (β), the diversity of which explains much of the variation in the radiative forcing from aerosol–cloud interactions (RFaci) in global climate models. This has made measuring β a key target for developing observational constraints of the aerosol forcing. While the aerosol burden of the clean, pre-industrial atmosphere has been demonstrated as a key uncertainty for the aerosol forcing, here we show that the behaviour of clouds under these clean conditions is of equal importance for understanding the spread in radiative forcing estimates between models and observations. This means that the uncertainty in the aerosol impact on clouds is, counterintuitively, driven by situations with little aerosol. Discarding clean conditions produces a close agreement between different model and observational estimates of the cloud response to aerosol but does not provide a strong constraint on the RFaci. This makes constraining aerosol behaviour in clean conditions an important goal for future observational studies.

With the advent of spaceborne spectroradiometers in a geostationary constellation, measuring high spectral resolution ultraviolet–visible (UV-VIS) and selected near-/shortwave-infrared (NIR/SWIR) radiances can enable the probing of the life cycle of key atmospheric trace gases and aerosols at higher temporal resolutions over the globe. The UV-VIS measurements are important for retrieving several key trace gases (e.g., O3, SO2, NO2, and HCHO) and particularly for deriving aerosol characteristics (e.g., aerosol absorption and vertical profile). This study examines the merit of simultaneous retrievals of trace gases and aerosols using a ground-based spectroradiometer covering the UV-NIR to monitor their physicochemical processes and to obtain reliable aerosol information for various applications. During the 2019 pre-monsoon season over northern Thailand, we deployed a ground-based SMART–s (Spectral Measurements for Atmospheric Radiative Transfer–spectroradiometer) instrument, which is an extended-range Pandora with reliable radiometric calibration in the 330–820 nm range, to retrieve remotely sensed chemical and aerosol properties for the first time near biomass burning sources. The high spectral resolution (∼ 1.0 nm full width half maximum with ∼ 3.7 × oversampling) of sun and sky measurements from SMART–s provides several key trace gases (e.g., O3, NO2, and H2O) and aerosol properties covering the UV where significant light absorption occurs by the carbonaceous particles. During the measurement period, highly correlated total column amounts of NO2 and aerosol optical thickness (τaer) retrieved from SMART–s (correlation coefficient, R=0.74) indicated their common emissions from biomass burning events. The SMART–s retrievals of the spectral single scattering albedo (ω0) of smoke aerosols showed an abrupt decrease in the UV, which is an important parameter dictating photochemical processes in the atmosphere. The values of ω0 and column precipitable water vapor (H2O) gradually increase with the mixing of biomass burning smoke particles and higher water vapor concentrations when approaching the monsoon season. The retrieved ω0 and weighted mean radius of fine-mode aerosols from SMART–s showed positive correlations with the H2O (R=0.81 for ω0 at 330 nm and 0.56 for the volume-weighted mean radius), whereas the real part of the refractive index of fine-mode aerosol (nf) showed negative correlations (R=-0.61 at 330 nm), which suggest that aerosol aging processes including hygroscopic growth (e.g., humidification and cloud processing) can be a major factor affecting the temporal trends of aerosol optical properties. Retrieved nf and ω0 were closer to those of the water droplet (i.e., nf of about 1.33 and ω0 of about 1.0) under lower amounts of NO2 during the measurement period; considering that the NO2 amounts in the smoke may indicate the aging of the plume after emission due to its short lifetime, the tendency is also consistent with active hygroscopic processes of the aerosols over this area. Retrieved UV aerosol properties from SMART–s generally support the assumed smoke aerosol models (i.e., the spectral shape of aerosol absorption) used in NASA's current satellite algorithms, and their spectral ω0 retrievals from ground and satellites showed good agreements (R = 0.73–0.79). However, temporal and spectral variabilities in the aerosol absorption properties in the UV emphasize the importance of a realistic optical model of aerosols for further improvements in satellite retrievals.