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In May–June 2019, smoke plumes from wildfires in Alberta, Canada, were advected all the way to Europe. To analyze the evolution of the plumes and to estimate the amount of smoke aerosols transported to Europe, retrievals from the spaceborne lidar CALIOP (Cloud-Aerosol LIdar with Orthogonal Polarization) were used. The plumes were located with the help of a trajectory analysis, and the masses of smoke aerosols were retrieved from the CALIOP observations. The accuracy of the CALIOP mass retrievals was compared with the accuracy of ground-based lidars/ceilometer near the source in North America and after the long-range transport in Europe. Overall, CALIOP and the ground-based lidars/ceilometer produced comparable results. Over North America the CALIOP layer mean mass was 30 % smaller than the ground-based estimates, whereas over southern Europe that difference varied between 12 % and 43 %. Finally, the CALIOP mass retrievals were compared with simulated aerosol concentrations from two reanalysis models: MERRA-2 (Modern-Era Retrospective analysis for Research and Applications, Version 2) and CAMS (Copernicus Atmospheric Monitoring System). The simulated total column aerosol optical depths (AODs) and the total column mass concentration of smoke agreed quite well with CALIOP observations, but the comparison of the layer mass concentration of smoke showed significant discrepancies. The amount of smoke aerosols in the model simulations was consistently smaller than in the CALIOP retrievals. These results highlight the limitations of such models and more specifically their limitation to reproduce properly the smoke vertical distribution. They indicate that CALIOP is a useful tool monitoring smoke plumes over secluded areas, whereas reanalysis models have difficulties in representing the aerosol mass in these plumes. This study shows the advantages of spaceborne aerosol lidars, e.g., being of paramount importance to monitor smoke plumes, and reveals the urgent need of future lidar missions in space. [ABSTRACT FROM AUTHOR]

Biomass burning aerosol impacts aspects of the atmosphere and Earth system through direct and semi-direct effects, as well as influencing air quality. Despite its importance, the representation of biomass burning aerosol is not always accurate in numerical weather prediction and climate models or reanalysis products. Using observations collected as part of the Cloud, Aerosol and Monsoon Processes Philippines Experiment (CAMP 2 Ex) in August through October of 2019, aerosol concentration and optical properties are evaluated within the Goddard Earth Observing System (GEOS) and its underlying aerosol module, GOCART. In the operational configuration, GEOS assimilates aerosol optical depth observations at 550 nm from AERONET and MODIS to constrain aerosol fields. Particularly for biomass burning aerosol, without the assimilation of aerosol optical depth, aerosol extinction is underestimated compared to observations collected in the Philippines region during the CAMP 2 Ex campaign. The assimilation process adds excessive amounts of carbon to account for the underestimated extinction, resulting in positive biases in the mass of black and organic carbon, especially within the boundary layer, relative to in situ observations from the Langley Aerosol Research Group Experiment. Counteracting this, GEOS is deficient in sulfate and nitrate aerosol just above the boundary layer. Aerosol extinction within GEOS is a function of the mass of different aerosol species, the ambient relative humidity, the assumed spectral optical properties, and particle size distribution per species. The relationship between dry and ambient extinction in GEOS reveals that hygroscopic growth is too high within the model for biomass burning aerosol. An additional concern lies in the assumed particle size distribution for GEOS, which has a single mode radius that is too small for organic carbon. Variability in the observed particle size distribution for biomass burning aerosol within a single flight also illuminates the fact that a single assumed particle size distribution is not sufficient and that for a proper representation, a more advanced aerosol module within GEOS may be necessary. [ABSTRACT FROM AUTHOR]

The uptake of water by atmospheric aerosols has a pronounced effect on particle light scattering properties, which in turn are strongly dependent on the ambient relative humidity (RH). Earth system models need to account for the aerosol water uptake and its influence on light scattering in order to properly capture the overall radiative effects of aerosols. Here we present a comprehensive model–measurement evaluation of the particle light scattering enhancement factor f (RH), defined as the particle light scattering coefficient at elevated RH (here set to 85 %) divided by its dry value. The comparison uses simulations from 10 Earth system models and a global dataset of surface-based in situ measurements. In general, we find a large diversity in the magnitude of predicted f (RH) amongst the different models, which can not be explained by the site types. Based on our evaluation of sea salt scattering enhancement and simulated organic mass fraction, there is a strong indication that differences in the model parameterizations of hygroscopicity and model chemistry are driving at least some of the observed diversity in simulated f (RH). Additionally, a key point is that defining dry conditions is difficult from an observational point of view and, depending on the aerosol, may influence the measured f (RH). The definition of dry also impacts our model evaluation, because several models exhibit significant water uptake between RH = 0 % and 40 %. The multisite average ratio between model outputs and measurements is 1.64 when RH = 0 % is assumed as the model dry RH and 1.16 when RH = 40 % is the model dry RH value. The overestimation by the models is believed to originate from the hygroscopicity parameterizations at the lower RH range which may not implement all phenomena taking place (i.e., not fully dried particles and hysteresis effects). This will be particularly relevant when a location is dominated by a deliquescent aerosol such as sea salt. Our results emphasize the need to consider the measurement conditions in such comparisons and recognize that measurements referred to as dry may not be dry in model terms. Recommendations for future model–measurement evaluation and model improvements are provided. [ABSTRACT FROM AUTHOR]

Satellite observations of the ultraviolet aerosol index (UVAI) are sensitive to absorption of solar radiation by aerosols; this absorption affects photolysis frequencies and radiative forcing. We develop a global simulation of the UVAI using the 3-D chemical transport model GEOSChem coupled with the Vector Linearized Discrete Ordinate Radiative Transfer model (VLIDORT). The simulation is applied to interpret UVAI observations from the Ozone Monitoring Instrument (OMI) for the year 2007. Simulated and observed values are highly consistent in regions where mineral dust dominates the UVAI, but a large negative bias (-0.32 to -0.97) exists between simulated and observed values in biomass burning regions. We determine effective optical properties for absorbing organic aerosol, known as brown carbon (BrC), and implement them into GEOS-Chem to better represent observed UVAI values over biomass burning regions. The inclusion of absorbing BrC decreases the mean bias between simulated and OMI UVAI values from -0.57 to -0.09 over West Africa in January, from -0.32 to +0.0002 over South Asia in April, from -0.97 to -0.22 over southern Africa in July, and from -0.50 to +0.33 over South America in September. The spectral dependence of absorption after including BrC in the model is broadly consistent with reported observations for biomass burning aerosol, with absorbing Ångström exponent (AAE) values ranging from 2.9 in the ultraviolet (UV) to 1.3 across the UV-Near IR spectrum. We assess the effect of the additional UV absorption by BrC on atmospheric photochemistry by examining tropospheric hydroxyl radical (OH) concentrations in GEOS-Chem. The inclusion of BrC decreases OH by up to 30% over South America in September, up to 20% over southern Africa in July, and up to 15% over other biomass burning regions. Global annual mean OH concentrations in GEOS-Chem decrease due to the presence of absorbing BrC, increasing the methyl chloroform lifetime from 5.62 to 5.68 years, thus reducing the bias against observed values. We calculate the direct radiative effect (DRE) of BrC using GEOS-Chem coupled with the radiative transfer model RRTMG (GC-RT). Treating organic aerosol as containing more strongly absorbing BrC changes the global annual mean all-sky top of atmosphere (TOA) DRE by +0.03 W m-2 and all-sky surface DRE by -0.08 W m-2. Regional changes of up to +0.3 W m-2 at TOA and down to -1.5 W m-2 at the surface are found over major biomass burning regions. [ABSTRACT FROM AUTHOR]