ALBERT

Description: The spatial distribution and properties of submicron organic aerosol (OA) are among the key sources of uncertainty in our understanding of aerosol effects on climate. Uncertainties are particularly large over remote regions of the free troposphere and Southern Ocean, where very few data have been available and where OA predictions from AeroCom Phase II global models span 2 to 3 orders of magnitude, greatly exceeding the model spread over source regions. The (nearly) pole-to-pole vertical distribution of non-refractory aerosols was measured with an aerosol mass spectrometer onboard the NASA DC-8 aircraft as part of the Atmospheric Tomography (ATom) mission during the Northern Hemisphere summer (August 2016) and winter (February 2017). This study presents the first extensive characterization of OA mass concentrations and their level of oxidation in the remote atmosphere. OA and sulfate are the major contributors by mass to submicron aerosols in the remote troposphere, together with sea salt in the marine boundary layer. Sulfate was dominant in the lower stratosphere. OA concentrations have a strong seasonal and zonal variability, with the highest levels measured in the lower troposphere in the summer and over the regions influenced by biomass burning from Africa (up to 10 µg sm−3). Lower concentrations (∼0.1–0.3 µg sm−3) are observed in the northern middle and high latitudes and very low concentrations (

Description: The radiative forcing of the aerosol–radiation interaction can be decomposed into clear-sky and cloudy-sky portions. Two sets of multi-model simulations within Aerosol Comparisons between Observations and Models (AeroCom), combined with observational methods, and the time evolution of aerosol emissions over the industrial era show that the contribution from cloudy-sky regions is likely weak. A mean of the simulations considered is 0.01±0.1 W m−2. Multivariate data analysis of results from AeroCom Phase II shows that many factors influence the strength of the cloudy-sky contribution to the forcing of the aerosol–radiation interaction. Overall, single-scattering albedo of anthropogenic aerosols and the interaction of aerosols with the short-wave cloud radiative effects are found to be important factors. A more dedicated focus on the contribution from the cloud-free and cloud-covered sky fraction, respectively, to the aerosol–radiation interaction will benefit the quantification of the radiative forcing and its uncertainty range.

Description: Aerosols from biomass burning (BB) emissions are poorly constrained in global and regional models, resulting in a high level of uncertainty in understanding their impacts. In this study, we compared six BB aerosol emission datasets for 2008 globally as well as in 14 regions. The six BB emission datasets are (1) GFED3.1 (Global Fire Emissions Database version 3.1), (2) GFED4s (GFED version 4 with small fires), (3) FINN1.5 (FIre INventory from NCAR version 1.5), (4) GFAS1.2 (Global Fire Assimilation System version 1.2), (5) FEER1.0 (Fire Energetics and Emissions Research version 1.0), and (6) QFED2.4 (Quick Fire Emissions Dataset version 2.4). The global total emission amounts from these six BB emission datasets differed by a factor of 3.8, ranging from 13.76 to 51.93 Tg for organic carbon and from 1.65 to 5.54 Tg for black carbon. In most of the regions, QFED2.4 and FEER1.0, which are based on satellite observations of fire radiative power (FRP) and constrained by aerosol optical depth (AOD) data from the Moderate Resolution Imaging Spectroradiometer (MODIS), yielded higher BB aerosol emissions than the rest by a factor of 2–4. By comparison, the BB aerosol emissions estimated from GFED4s and GFED3.1, which are based on satellite burned-area data, without AOD constraints, were at the low end of the range. In order to examine the sensitivity of model-simulated AOD to the different BB emission datasets, we ingested these six BB emission datasets separately into the same global model, the NASA Goddard Earth Observing System (GEOS) model, and compared the simulated AOD with observed AOD from the AErosol RObotic NETwork (AERONET) and the Multiangle Imaging SpectroRadiometer (MISR) in the 14 regions during 2008. In Southern Hemisphere Africa (SHAF) and South America (SHSA), where aerosols tend to be clearly dominated by smoke in September, the simulated AOD values were underestimated in almost all experiments compared to MISR, except for the QFED2.4 run in SHSA. The model-simulated AOD values based on FEER1.0 and QFED2.4 were the closest to the corresponding AERONET data, being, respectively, about 73 % and 100 % of the AERONET observed AOD at Alta Floresta in SHSA and about 49 % and 46 % at Mongu in SHAF. The simulated AOD based on the other four BB emission datasets accounted for only ∼50 % of the AERONET AOD at Alta Floresta and ∼20 % at Mongu. Overall, during the biomass burning peak seasons, at most of the selected AERONET sites in each region, the AOD values simulated with QFED2.4 were the highest and closest to AERONET and MISR observations, followed closely by FEER1.0. However, the QFED2.4 run tends to overestimate AOD in the region of SHSA, and the QFED2.4 BB emission dataset is tuned with the GEOS model. In contrast, the FEER1.0 BB emission dataset is derived in a more model-independent fashion and is more physically based since its emission coefficients are independently derived at each grid box. Therefore, we recommend the FEER1.0 BB emission dataset for aerosol-focused hindcast experiments in the two biomass-burning-dominated regions in the Southern Hemisphere, SHAF, and SHSA (as well as in other regions but with lower confidence). The differences between these six BB emission datasets are attributable to the approaches and input data used to derive BB emissions, such as whether AOD from satellite observations is used as a constraint, whether the approaches to parameterize the fire activities are based on burned area, FRP, or active fire count, and which set of emission factors is chosen.

Description: Ambient air pollution from ozone and fine particulate matter is associated with premature mortality. As emissions from one continent influence air quality over others, changes in emissions can also influence human health on other continents. We estimate global air-pollution-related premature mortality from exposure to PM2.5 and ozone and the avoided deaths due to 20 % anthropogenic emission reductions from six source regions, North America (NAM), Europe (EUR), South Asia (SAS), East Asia (EAS), Russia–Belarus–Ukraine (RBU), and the Middle East (MDE), three global emission sectors, power and industry (PIN), ground transportation (TRN), and residential (RES), and one global domain (GLO), using an ensemble of global chemical transport model simulations coordinated by the second phase of the Task Force on Hemispheric Transport of Air Pollutants (TF HTAP2), and epidemiologically derived concentration response functions. We build on results from previous studies of TF HTAP by using improved atmospheric models driven by new estimates of 2010 anthropogenic emissions (excluding methane), with more source and receptor regions, new consideration of source sector impacts, and new epidemiological mortality functions. We estimate 290 000 (95 % confidence interval (CI): 30 000, 600 000) premature O3-related deaths and 2.8 million (0.5 million, 4.6 million) PM2.5-related premature deaths globally for the baseline year 2010. While 20 % emission reductions from one region generally lead to more avoided deaths within the source region than outside, reducing emissions from MDE and RBU can avoid more O3-related deaths outside of these regions than within, and reducing MDE emissions also avoids more PM2.5-related deaths outside of MDE than within. Our findings that most avoided O3-related deaths from emission reductions in NAM and EUR occur outside of those regions contrast with those of previous studies, while estimates of PM2.5-related deaths from NAM, EUR, SAS, and EAS emission reductions agree well. In addition, EUR, MDE, and RBU have more avoided O3-related deaths from reducing foreign emissions than from domestic reductions. For six regional emission reductions, the total avoided extra-regional mortality is estimated as 6000 (−3400, 15 500) deaths per year and 25 100 (8200, 35 800) deaths per year through changes in O3 and PM2.5, respectively. Interregional transport of air pollutants leads to more deaths through changes in PM2.5 than in O3, even though O3 is transported more on interregional scales, since PM2.5 has a stronger influence on mortality. For NAM and EUR, our estimates of avoided mortality from regional and extra-regional emission reductions are comparable to those estimated by regional models for these same experiments. In sectoral emission reductions, TRN emissions account for the greatest fraction (26–53 % of global emission reduction) of O3-related premature deaths in most regions, in agreement with previous studies, except for EAS (58 %) and RBU (38 %) where PIN emissions dominate. In contrast, PIN emission reductions have the greatest fraction (38–78 % of global emission reduction) of PM2.5-related deaths in most regions, except for SAS (45 %) where RES emission dominates, which differs with previous studies in which RES emissions dominate global health impacts. The spread of air pollutant concentration changes across models contributes most to the overall uncertainty in estimated avoided deaths, highlighting the uncertainty in results based on a single model. Despite uncertainties, the health benefits of reduced intercontinental air pollution transport suggest that international cooperation may be desirable to mitigate pollution transported over long distances.

Description: Atmospheric aerosols from anthropogenic and natural sources reach the polar regions through long-range transport and affect the local radiation balance. Such transport is, however, poorly constrained in present-day global climate models, and few multi-model evaluations of polar anthropogenic aerosol radiative forcing exist. Here we compare the aerosol optical depth (AOD) at 550 nm from simulations with 16 global aerosol models from the AeroCom Phase II model intercomparison project with available observations at both poles. We show that the annual mean multi-model median is representative of the observations in Arctic, but that the intermodel spread is large. We also document the geographical distribution and seasonal cycle of the AOD for the individual aerosol species: black carbon (BC) from fossil fuel and biomass burning, sulfate, organic aerosols (OAs), dust, and sea-salt. For a subset of models that represent nitrate and secondary organic aerosols (SOAs), we document the role of these aerosols at high latitudes.The seasonal dependence of natural and anthropogenic aerosols differs with natural aerosols peaking in winter (sea-salt) and spring (dust), whereas AOD from anthropogenic aerosols peaks in late spring and summer. The models produce a median annual mean AOD of 0.07 in the Arctic (defined here as north of 60° N). The models also predict a noteworthy aerosol transport to the Antarctic (south of 70° S) with a resulting AOD varying between 0.01 and 0.02. The models have estimated the shortwave anthropogenic radiative forcing contributions to the direct aerosol effect (DAE) associated with BC and OA from fossil fuel and biofuel (FF), sulfate, SOAs, nitrate, and biomass burning from BC and OA emissions combined. The Arctic modelled annual mean DAE is slightly negative (−0.12 W m−2), dominated by a positive BC FF DAE in spring and a negative sulfate DAE in summer. The Antarctic DAE is governed by BC FF. We perform sensitivity experiments with one of the AeroCom models (GISS modelE) to investigate how regional emissions of BC and sulfate and the lifetime of BC influence the Arctic and Antarctic AOD. A doubling of emissions in eastern Asia results in a 33 % increase in Arctic AOD of BC. A doubling of the BC lifetime results in a 39 % increase in Arctic AOD of BC. However, these radical changes still fall within the AeroCom model range.

Description: 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.

Description: Topic 3 of the Model Inter-Comparison Study for Asia (MICS-Asia) Phase III examines how online coupled air quality models perform in simulating high aerosol pollution in the North China Plain region during wintertime haze events and evaluates the importance of aerosol radiative and microphysical feedbacks. A comprehensive overview of the MICS-Asia III Topic 3 study design, including descriptions of participating models and model inputs, the experimental designs, and results of model evaluation, are presented. Six modeling groups from China, Korea and the United States submitted results from seven applications of online coupled chemistry–meteorology models. Results are compared to meteorology and air quality measurements, including data from the Campaign on Atmospheric Aerosol Research Network of China (CARE-China) and the Acid Deposition Monitoring Network in East Asia (EANET). The correlation coefficients between the multi-model ensemble mean and the CARE-China observed near-surface air pollutants range from 0.51 to 0.94 (0.51 for ozone and 0.94 for PM2.5) for January 2010. However, large discrepancies exist between simulated aerosol chemical compositions from different models. The coefficient of variation (SD divided by the mean) can reach above 1.3 for sulfate in Beijing and above 1.6 for nitrate and organic aerosols in coastal regions, indicating that these compositions are less consistent from different models. During clean periods, simulated aerosol optical depths (AODs) from different models are similar, but peak values differ during severe haze events, which can be explained by the differences in simulated inorganic aerosol concentrations and the hygroscopic growth efficiency (affected by varied relative humidity). These differences in composition and AOD suggest that future models can be improved by including new heterogeneous or aqueous pathways for sulfate and nitrate formation under hazy conditions, a secondary organic aerosol (SOA) formation chemical mechanism with new volatile organic compound (VOCs) precursors, yield data and approaches, and a more detailed evaluation of the dependence of aerosol optical properties on size distribution and mixing state. It was also found that using the ensemble mean of the models produced the best prediction skill. While this has been shown for other conditions (for example, the prediction of high-ozone events in the US (McKeen et al., 2005)), this is to our knowledge the first time it has been shown for heavy haze events.

Description: An assessment of global particulate nitrate and ammonium aerosol based on simulations from nine models participating in the Aerosol Comparisons between Observations and Models (AeroCom) phase III study is presented. A budget analysis was conducted to understand the typical magnitude, distribution, and diversity of the aerosols and their precursors among the models. To gain confidence regarding model performance, the model results were evaluated with various observations globally, including ground station measurements over North America, Europe, and east Asia for tracer concentrations and dry and wet depositions, as well as with aircraft measurements in the Northern Hemisphere mid-to-high latitudes for tracer vertical distributions. Given the unique chemical and physical features of the nitrate occurrence, we further investigated the similarity and differentiation among the models by examining (1) the pH-dependent NH3 wet deposition; (2) the nitrate formation via heterogeneous chemistry on the surface of dust and sea salt particles or thermodynamic equilibrium calculation including dust and sea salt ions; and (3) the nitrate coarse-mode fraction (i.e., coarse/total). It is found that HNO3, which is simulated explicitly based on full O3-HOx-NOx-aerosol chemistry by all models, differs by up to a factor of 9 among the models in its global tropospheric burden. This partially contributes to a large difference in NO3−, whose atmospheric burden differs by up to a factor of 13. The atmospheric burdens of NH3 and NH4+ differ by 17 and 4, respectively. Analyses at the process level show that the large diversity in atmospheric burdens of NO3−, NH3, and NH4+ is also related to deposition processes. Wet deposition seems to be the dominant process in determining the diversity in NH3 and NH4+ lifetimes. It is critical to correctly account for contributions of heterogeneous chemical production of nitrate on dust and sea salt, because this process overwhelmingly controls atmospheric nitrate production (typically 〉 80 %) and determines the coarse- and fine-mode distribution of nitrate aerosol.

Description: Haze has been severely affecting the densely populated areas in China recently. While many of the efforts have been devoted to investigating the impact of local anthropogenic emission, limited attention has been paid to the contribution from long-range transport. In this study, we apply simulations from six participating models supplied through the Task Force on Hemispheric Transport of Air Pollution phase 2 (HTAP2) exercise to investigate the long-range transport impact of Europe (EUR) and Russia–Belarus–Ukraine (RBU) on the surface air quality in eastern Asia (EAS), with special focus on their contributions during the haze episodes in China. The impact of 20 % anthropogenic emission perturbation from the source region is extrapolated by a factor of 5 to estimate the full impact. We find that the full impacts from EUR and RBU are 0.99 µg m−3 (3.1 %) and 1.32 µg m−3 (4.1 %) during haze episodes, while the annual averaged full impacts are only 0.35 µg m−3 (1.7 %) and 0.53 µg m−3 (2.6 %). By estimating the aerosol response within and above the planetary boundary layer (PBL), we find that long-range transport from EUR within the PBL contributes to 22–38 % of the total column density of aerosol response in EAS. Comparison with the HTAP phase 1 (HTAP1) assessment reveals that from 2000 to 2010, the long-range transport from Europe to eastern Asia has decreased significantly by a factor of 2–10 for surface aerosol mass concentration due to the simultaneous emission reduction in source regions and emission increase in the receptor region. We also find the long-range transport from the Europe and RBU regions increases the number of haze events in China by 0.15 % and 0.11 %, and the North China Plain and southeastern China has 1–3 extra haze days (

Description: Topic 3 of the Model Inter-Comparison Study for Asia (MICS-Asia) Phase III examines how online coupled air quality models perform in simulating wintertime haze events in the North China Plain region and evaluates the importance of aerosol radiative feedbacks. This paper discusses the estimates of aerosol radiative forcing, aerosol feedbacks, and possible causes for the differences among the participating models. Over the Beijing–Tianjin–Hebei (BTH) region, the ensemble mean of estimated aerosol direct radiative forcing (ADRF) at the top of atmosphere, inside the atmosphere, and at the surface are −1.1, 7.7, and −8.8 W m−2 during January 2010, respectively. Subdivisions of direct and indirect aerosol radiative forcing confirm the dominant role of direct forcing. During severe haze days (17–19 January 2010), the averaged reduction in near-surface temperature for the BTH region can reach 0.3–1.6 ∘C. The responses of wind speeds at 10 m (WS10) inferred from different models show consistent declines in eastern China. For the BTH region, aerosol–radiation feedback-induced daytime changes in PM2.5 concentrations during severe haze days range from 6.0 to 12.9 µg m−3 (