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An increase in the sulfate aerosols observed in the period 1–6 April 2014 over Austria is analyzed using in situ measurements at an Austrian air quality background station, lidar measurements at the closest EARLINET stations around Austria, CAMS near-real-time data, and particle dispersion modeling using FLEXPART, a Lagrangian transport model. In situ measurements of SO2 , PM 2.5 , PM 10 , and O3 were performed at the air quality background station Pillersdorf, Austria (EMEP station AT30, 48 ∘ 43 ′ N, 15 ∘ 55 ′ E). A CAMS aerosol mixing ratio analysis for Pillersdorf and the lidar stations Leipzig, Munich, Garmisch, and Bucharest indicates the presence of an event of aerosol transport, with sulfate and dust as principal components. For the sulfate layers identified at Pillersdorf from the CAMS analysis, backward- and forward-trajectory analyses were performed, associating lidar stations with the trajectories. The lidar measurements for the period corresponding to trajectory overpass of associated stations were analyzed, obtaining the aerosol layers, the optical properties, and the aerosol types. The potential sources of transported aerosols were determined for Pillersdorf and the lidar stations using the source–receptor sensitivity computed with FLEXPART, combined with the MACCity source inventory. A comparative analysis for Pillersdorf and the trajectory-associated lidar stations showed consistent aerosol layers, optical properties and types, and potential sources. A complex pattern of contributions to sulfate over Austria was found in this paper. For the lower layers (below 2000 m) of sulfate, it was found that central Europe was the main source of sulfate. Medium to smaller contributions come from sources in eastern Europe, northwest Africa, and the eastern US. For the middle-altitude layers (between 2000 and 5000 m), sources from central Europe (northern Italy, Serbia, Hungary) contribute with similar emissions. Northwest Africa and the eastern US also have important contributions. For the high-altitude layers (above 5000 m), the main contributions come from northwest Africa, but sources from the southern and eastern US also contribute significantly. No contributions from Europe are seen for these layers. The methodology used in this paper can be used as a general tool to correlate measurements at in situ stations and EARLINET lidar stations around these in situ stations. [ABSTRACT FROM AUTHOR]

This study estimates the health risk due to PM 2.5 and ADE primarily in 4 regions across Northern Hemisphere during 2013-2017. Mortality in China due to PM 2.5 dipped from 1.15 million (95%CI (Confidence Interval) 0.64-1.6 million) to 1.02 million (95%CI 0.59-1.49 million) during 2013-2017 as a result of reduction in PM 2.5 population weighted concentration (PWC) from 29.26 μg/m 3 to 22.05 μg/m 3 while India overtook China in terms of death due to PM 2.5 which increased to 1.16 million (95%CI 0.72-1.67 million) from 1.07 million (95%CI 0.62-1.53 million) as a result of increase in PWC from 38.18 to 44.47 μg/m 3 . The years of life lost per person (YLL/person) due to PM 2.5 was still observed to be high in China with 5.58 YLL/person followed by India (4.13), Europe (2.19) and US (0.46) in 2017. Aerosols such as PM 2.5 have the capability to scatter or absorb solar radiation resulting in perturbation of ground meteorology which further affects dispersion of pollutants and it's resultant health impacts. ADE resulted in 7.27% of total or 77,866 deaths in India during 2013 which increased to 8.05% or 93,575 deaths in 2017 which was highest among all regions while in China ADE deaths reduced from 59,529 (5.15% of total) to 40,470 (3.94% of total) deaths during the same period, other regions too reported reduction in ADE deaths with US reporting 906 (-1.27%) lower deaths while Europe also reported 785 (-0.46%) lower deaths in 2017 as compared to 2013. ADE resulted in increased YLL/person in India from 0.29 to 0.33 during 2013-2017 while it was observed to reduce in all other regions, in China it reduced from 0.37 to 0.22 likewise YLL/person also reduced in US from 0.04 to 0.01 and in Europe from 0.01 to 0.002., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2020 Elsevier Ltd. All rights reserved.)

In this article, we describe multiannual variations of the atmospheric aerosol optical depth values in the widely understood area of the Baltic Sea. We present the trends in the changes and depict unusual aerosol situations. As a result of analyses, we focus on 2019, since unusually high values of aerosol optical depth were recorded in several stations around the Baltic. We match the high aerosol levels with an unusually high number of wildfires across Europe in spring and summer, which emitted large quantities of aerosols into the atmosphere that were distributed over vast European areas in part by the wind. We then connect this case with the climate change consequences. Since aerosols influence the radiative budget of the planet by directly affecting the atmospheric radiation budget, it is obvious that human well-being is in danger due to wildfires, as well as from the atmospheric perspective. Climate change will lead to more frequent fires; thus, humans need to develop solutions to decrease the risk of fire outbreaks. [ABSTRACT FROM AUTHOR]

E-cigarette use has become increasingly popular, especially among the young. Its long-term influence upon health is unknown. Aim of this review has been to present the current state of knowledge about the impact of e-cigarette use on health, with an emphasis on Central and Eastern Europe. During the preparation of this narrative review, the literature on e-cigarettes available within the network PubMed was retrieved and examined. In the final review, 64 research papers were included. We specifically assessed the construction and operation of the e-cigarette as well as the chemical composition of the e-liquid; the impact that vapor arising from the use of e-cigarette explored in experimental models in vitro; and short-term effects of use of e-cigarettes on users' health. Among the substances inhaled by the e-smoker, there are several harmful products, such as: formaldehyde, acetaldehyde, acroleine, propanal, nicotine, acetone, o-methyl-benzaldehyde, carcinogenic nitrosamines. Results from experimental animal studies indicate the negative impact of e-cigarette exposure on test models, such as ascytotoxicity, oxidative stress, inflammation, airway hyper reactivity, airway remodeling, mucin production, apoptosis, and emphysematous changes. The short-term impact of e-cigarettes on human health has been studied mostly in experimental setting. Available evidence shows that the use of e-cigarettes may result in acute lung function responses (e.g., increase in impedance, peripheral airway flow resistance) and induce oxidative stress. Based on the current available evidence, e-cigarette use is associated with harmful biologic responses, although it may be less harmful than traditional cigarettes. Int J Occup Med Environ Health 2017;30(3):329-344. [ABSTRACT FROM AUTHOR]

Recent years have seen an increase in the use of wood for energy production of over 30 %, and this trend is expected to continue due to the current energy crisis and geopolitical instability. At present, residential wood burning (RWB) is one of the most important sources of organic aerosols (OAs) and black carbon (BC), posing a significant risk to air quality and health. Simultaneously, as a substantial aerosol source, RWB also holds relevance in the context of aerosol radiative effects and climate. While BC is recognized for its large light absorption cross-section, the role of OAs in light absorption is still under evaluation due to their heterogeneous composition and source-dependent optical properties. Existing studies that characterize wood-burning aerosol emissions in Europe primarily concentrate on urban and background sites and focus on BC properties. Despite the significant RWB emissions in rural areas, these locations have received comparatively less attention. The present scenario underscores the imperative for an improved understanding of RWB pollution, aerosol optical properties, and their subsequent connection to climate impacts, particularly in rural areas. We have characterized atmospheric aerosol particles from a central European rural site during wintertime in the village of Retje in Loški Potok, Slovenia, from 1 December 2017 to 7 March 2018. The village experienced extremely high aerosol concentrations produced by RWB and near-ground temperature inversion. The isolated location of the site and the substantial local emissions made it an ideal laboratory-like place for characterizing RWB aerosols with low influence from non-RWB sources under ambient conditions. The mean mass concentrations of OA and BC were 35 µgm-3 (max⁡=270 µgm-3) and 3.1 µgm-3 (max⁡=24 µgm-3), respectively. The mean total particle number concentration (10–600 nm) was 9.9×103 particles cm -3 (max⁡=59×103 particles cm -3). The mean total light absorption coefficients at 370 and 880 nm measured by an AE33 Aethalometer were 120 and 22 Mm -1 and had maximum values of 1100 and 180 Mm -1 , respectively. The aerosol concentrations and absorption coefficients measured during the campaign in Loški Potok were significantly larger than reported values for several urban areas in the region with larger populations and a larger extent of aerosol sources. Here, considerable contributions from brown carbon (BrC) to the total light absorption were identified, reaching up to 60 % and 48 % in the near-UV (370 nm) and blue (470 nm) wavelengths. These contributions are up to 3 times higher than values reported for other sites impacted by wood-burning emissions. The calculated mass absorption cross-section and the absorption Ångström exponent for RWB OA were MAC OA,370nm=2.4 m 2 g -1 , and AAE BrC,370-590nm=3.9 , respectively. Simple-forcing-efficiency (SFE) calculations were performed as a sensitivity analysis to evaluate the climate impact of the RWB aerosols produced at the study site by integrating the optical properties measured during the campaign. The SFE results show a considerable forcing capacity from the local RWB aerosols, with a high sensitivity to OA absorption properties and a more substantial impact over bright surfaces like snow, typical during the coldest season with higher OA emissions from RWB. Our study's results are highly significant regarding air pollution, optical properties, and climate impact. The findings suggest that there may be an underestimation of RWB emissions in rural Europe and that further investigation is necessary. [ABSTRACT FROM AUTHOR]

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]

Wildfires are a significant source of organic aerosol during summer, with major impacts on air quality and climate. However, studies in Europe suggest a surprisingly low (less than 10%) contribution of biomass burning organic aerosol to average summertime fine particulate matter levels. In this study we combine field measurements and atmospheric chemical transport modeling, to demonstrate that the contribution of wildfires to fine particle levels in Europe during summer is seriously underestimated. Our work suggests that the corresponding contribution has been underestimated by a factor of 4–7 and that wildfires were responsible for approximately half of the total OA in Europe during July 2022. This discrepancy with previous work is due to the rapid physicochemical transformation of these emissions to secondary oxidized organic aerosol with an accompanying loss of its organic chemical fingerprints. These atmospheric reactions lead to a regionally distributed background organic aerosol that is responsible for a significant fraction of the health-related impacts caused by fine particles in Europe and probably in other continents. These adverse health effects can occur hundreds or even thousands of kilometers away from the fires. We estimate that wildfire emissions are responsible for 15–22% of the deaths in Europe due to exposure to fine particulate matter during summer. [ABSTRACT FROM AUTHOR]

The European Aerosol Research Lidar Network (EARLINET), part of the Aerosols, Clouds and Trace gases Research Infrastructure (ACTRIS), organized an intensive observational campaign in May 2020, with the objective of monitoring the atmospheric state over Europe during the COVID-19 lockdown and relaxation period. Besides the standard operational processing of the lidar data in EARLINET, for seven EARLINET sites having collocated sun-photometric observations in the Aerosol Robotic Network (AERONET), a network exercise was held in order to derive profiles of the concentration and effective column size distributions of the aerosols in the atmosphere, by applying the GRASP/GARRLiC (from Generalized Aerosol Retrieval from Radiometer and Lidar Combined data – GARRLiC – part of the Generalized Retrieval of Atmosphere and Surface Properties – GRASP) inversion algorithm. The objective of this network exercise was to explore the possibility of identifying the anthropogenic component and of monitoring its spatial and temporal characteristics in the COVID-19 lockdown and relaxation period. While the number of cases is far from being statistically significant so as to provide a conclusive description of the atmospheric aerosols over Europe during this period, this network exercise was fundamental to deriving a common methodology for applying GRASP/GARRLiC to a network of instruments with different characteristics. The limits of the approach are discussed, in particular the missing information close to the ground in the lidar measurements due to the instrument geometry and the sensitivity of the GRASP/GARRLiC retrieval to the settings used, especially for cases with low aerosol optical depth (AOD) like the ones we show here. We found that this sensitivity is well-characterized in the GRASP/GARRLiC products, since it is included in their retrieval uncertainties. [ABSTRACT FROM AUTHOR]

The present work describes the implementation of the state of the art Cloud- J v7.3 photolysis rate calculation code in the EMEP MSC-W chemistry-transport model. Cloud- J calculates photolysis rates and accounts for cloud and aerosol optical properties at model run time, replacing the old system based on tabulated values. The performance of Cloud- J is evaluated against aerial photolysis rate observations made over the Pacific Ocean and against surface observations from three measurement sites in Europe. Numerical experiments are performed to investigate the sensitivity of the calculated photolysis rates to the spatial and temporal model resolution, input meteorology model, simulated ozone column, and cloud effect parameterization. These experiments indicate that the calculated photolysis rates are most sensitive to the choice of input meteorology model and cloud effect parameterization while also showing that surface ozone photolysis rates can vary by up to 20 % due to daily variations in total ozone column. Further analysis investigates the impact of Cloud- J on the oxidizing capacity of the troposphere, aerosol–photolysis interactions, and surface air quality predictions. Results find that the annual mean mass-weighted tropospheric hydroxyl concentration is increased by 26 %, while the photolytic impact of aerosols is mostly limited to large tropical biomass-burning regions. Overall, Cloud- J represents a major improvement over the tabulated system, leading to improved model performance for predicting carbon monoxide and daily maximum ozone surface concentrations. [ABSTRACT FROM AUTHOR]

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 space-borne lidar CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) were used. The plumes were located with the help of a trajectory analysis, and the mass 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 (AOD) 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 space-borne 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]

The recent COVID-19 pandemic affected various aspects of life. Several studies established the consequences of pandemic lockdown on air quality using satellite remote sensing. However, such studies have limitations, including low spatial resolution or incomplete spatial coverage. Therefore, in this paper, we propose a machine learning-based scheme to solve the pre-mentioned limitations by training an optimized space-time extra trees model for each year of the study period. The results have shown that our trained models reach a prediction accuracy up to 95% when predicting the missing values in the MODIS MCD19A2 Aerosol Optical Depth (AOD) product. The outcome of the mentioned scheme was a geo-harmonized atmospheric dataset for aerosol optical depth at 550 nm with 1 km spatial resolution and full coverage over Europe. As an application, we used the proposed machine learning based prediction approach in AOD levels analysis. We compared the mean AOD levels between the lockdown period from March to June in 2020 and the mean AOD values of the same period for the past 5 years. We found that AOD levels dropped over most European countries in 2020 but increased in several eastern and western countries. The Netherlands had the most significant average decrease in AOD levels (19%), while Spain had the highest average increase (10%). Moreover, we analyzed the relationship between the relative percentage difference of AOD and four meteorological variables. We found a positive correlation between AOD and relative humidity and a negative correlation between AOD and wind speed. The value of the proposed prediction scheme is further emphasized by taking into consideration that the reconstructed dataset can be used for future air quality studies concerning Europe. [ABSTRACT FROM AUTHOR]

Atmospheric aerosol particles are a complex combination of primary emitted sources (biogenic and anthropogenic) and secondary aerosol resulting from aging processes such as condensation, coagulation, and cloud processing. To better understand their sources, investigations have been focused on urban areas in the past, whereas rural-background stations are normally less impacted by surrounding anthropogenic sources. Therefore, they are predisposed for studying the impact of long-range transport of anthropogenic aerosols. Here, the chemical composition and organic aerosol (OA) sources of submicron aerosol particles measured by an aerosol chemical speciation monitor (ACSM) and a multi-angle absorption photometer (MAAP) were investigated at Melpitz from September 2016 to August 2017. The location of the station at the frontier between western and eastern Europe makes it the ideal place to investigate the impact of long-range transport over Europe. Indeed, the station is under the influence of less polluted air masses from westerly directions and more polluted continental air masses from eastern Europe. The OA dominated the submicron particle mass concentration and showed strong seasonal variability ranging from 39 % (in winter) to 58 % (in summer). It was followed by sulfate (15 % and 20 %) and nitrate (24 % and 11 %). The OA source identification was performed using the rolling positive matrix factorization (PMF) approach to account for the potential temporal changes in the source profile. It was possible to split OA into five factors with a distinct temporal variability and mass spectral signature. Three were associated with anthropogenic primary OA (POA) sources: hydrocarbon-like OA (HOA; 5.2 % of OA mass in winter and 6.8 % in summer), biomass burning OA (BBOA; 10.6 % and 6.1 %) and coal combustion OA (CCOA; 23 % and 8.7 %). Another two are secondary and processed oxygenated OA (OOA) sources: less oxidized OOA (LO-OOA; 28.4 % and 36.7 %) and more oxidized OOA (MO-OOA; 32.8 % and 41.8 %). Since equivalent black carbon (eBC) was clearly associated with the identified POA factors (sum of HOA, BBOA, and CCOA; R2= 0. 87), eBC's contribution to each of the POA factors was achieved using a multilinear regression model. Consequently, CCOA represented the main anthropogenic sources of carbonaceous aerosol (sum of OA and eBC) not only during winter (56 % of POA in winter) but also in summer (13 % of POA in summer), followed by BBOA (29 % and 69 % of POA in winter and summer, respectively) and HOA (15 % and 18 % of POA in winter and summer, respectively). A seasonal air mass cluster analysis was used to understand the geographical origins of the different aerosol types and showed that during both winter and summer time, PM 1 (PM with an aerodynamic diameter smaller than 1 µm) air masses with eastern influence were always associated with the highest mass concentration and the highest coal combustion fraction. Since during wintertime CCOA is a combination of domestic heating and power plant emissions, the summer contribution of CCOA emphasizes the critical importance of coal power plant emissions to rural-background aerosols and its impact on air quality, through long-range transportation. [ABSTRACT FROM AUTHOR]

Soot, or black carbon (BC), aerosol is a major climate forcer with severe health effects. The impacts depend strongly on particle number concentration, size and mixing state. This work reports on two field campaigns at nearby urban and rural sites, 65 km apart, in southern Sweden during late summer 2018. BC was measured using a single-particle soot photometer (SP2) and Aethalometers (AE33). Differences in BC concentrations between the sites are driven primarily by local traffic emissions. Equivalent and refractory BC mass concentrations at the urban site were on average a factor 2.2 and 2.5, with peaks during rush hour up to a factor ∼4 , higher than the rural background levels. The number fraction of particles containing a soot core was significantly higher in the city. BC particles at the urban site were on average smaller by mass and had less coating owing to fresh traffic emissions. The organic components of the fresh traffic plumes were similar in mass spectral signature to hydrocarbon-like organic aerosol (HOA), commonly associated with traffic. Despite the intense local traffic (∼ 30 000 vehicles passing per day), PM 1 , including organic aerosol, was dominated by aged continental air masses even at the curbside site. The fraction of thickly coated particles at the urban site was highly correlated with the mass concentrations of all measured chemical species of PM 1 , consistent with aged, internally mixed aerosol. Trajectory analysis for the whole year showed that air masses arriving at the rural site from eastern Europe contained approximately double the amount of BC compared to air masses from western Europe. Furthermore, the largest regional emissions of BC transported to the rural site, from the Malmö–Copenhagen urban area, are discernible above background levels only when precipitation events are excluded. We show that continental Europe and not the Malmö–Copenhagen region is the major contributor to the background BC mass concentrations in southern Sweden. [ABSTRACT FROM AUTHOR]

Aerosol optical depth (AOD) is one of the basic characteristics of atmospheric aerosol. A global ground-based network of sun and sky photometers, the Aerosol Robotic Network (AERONET) provides AOD data with low uncertainty. However, AERONET observations are sparse in space and time. To improve data density, we merged AERONET observations with a GEOS-Chem chemical transport model prediction using an optimal interpolation (OI) method. According to OI, we estimated AOD as a linear combination of observational data and a model forecast, with weighting coefficients chosen to minimize a mean-square error in the calculation, assuming a negligible error of AERONET AOD observations. To obtain weight coefficients, we used correlations between model errors in different grid points. In contrast with classical OI, where only spatial correlations are considered, we developed the spatial-temporal optimal interpolation (STOI) technique for atmospheric applications with the use of spatial and temporal correlation functions. Using STOI, we obtained estimates of the daily mean AOD distribution over Europe. To validate the results, we compared daily mean AOD estimated by STOI with independent AERONET observations for two months and three sites. Compared with the GEOS-Chem model results, the averaged reduction of the root-mean-square error of the AOD estimate based on the STOI method is about 25%. The study shows that STOI provides a significant improvement in AOD estimates. [ABSTRACT FROM AUTHOR]

Despite a large number of studies, out of all drivers of radiative forcing, the effect of aerosols has the largest uncertainty in global climate model radiative forcing estimates. There have been studies of aerosol optical properties in climate models, but the effects of particle number size distribution need a more thorough inspection. We investigated the trends and seasonality of particle number concentrations in nucleation, Aitken, and accumulation modes at 21 measurement sites in Europe and the Arctic. For 13 of those sites, with longer measurement time series, we compared the field observations with the results from five climate models, namely EC-Earth3, ECHAM-M7, ECHAM-SALSA, NorESM1.2, and UKESM1. This is the first extensive comparison of detailed aerosol size distribution trends between in situ observations from Europe and five earth system models (ESMs). We found that the trends of particle number concentrations were mostly consistent and decreasing in both measurements and models. However, for many sites, climate models showed weaker decreasing trends than the measurements. Seasonal variability in measured number concentrations, quantified by the ratio between maximum and minimum monthly number concentration, was typically stronger at northern measurement sites compared to other locations. Models had large differences in their seasonal representation, and they can be roughly divided into two categories: for EC-Earth and NorESM, the seasonal cycle was relatively similar for all sites, and for other models the pattern of seasonality varied between northern and southern sites. In addition, the variability in concentrations across sites varied between models, some having relatively similar concentrations for all sites, whereas others showed clear differences in concentrations between remote and urban sites. To conclude, although all of the model simulations had identical input data to describe anthropogenic mass emissions, trends in differently sized particles vary among the models due to assumptions in emission sizes and differences in how models treat size-dependent aerosol processes. The inter-model variability was largest in the accumulation mode, i.e. sizes which have implications for aerosol–cloud interactions. Our analysis also indicates that between models there is a large variation in efficiency of long-range transportation of aerosols to remote locations. The differences in model results are most likely due to the more complex effect of different processes instead of one specific feature (e.g. the representation of aerosol or emission size distributions). Hence, a more detailed characterization of microphysical processes and deposition processes affecting the long-range transport is needed to understand the model variability. [ABSTRACT FROM AUTHOR]

The abrupt reduction in human activities during the first lockdown of the COVID-19 pandemic created unprecedented atmospheric conditions. To quantify the changes in lower tropospheric air pollution, we conducted the BLUESKY aircraft campaign and measured vertical profiles of black carbon (BC) aerosol particles over western and southern Europe in May and June 2020. We compared the results to similar measurements of the EMeRGe EU campaign performed in July 2017 and found that the BC mass concentrations (MBC) were reduced by about 48%. For BC particle number concentrations, we found comparable reductions. Based on ECHAM/MESSy Atmospheric Chemistry (EMAC) chemistry-transport model simulations, we found differences in meteorological conditions and flight patterns responsible for about 7% of the MBC reductions. Accordingly 41% of MBC reductions can be attributed to reduced anthropogenic emissions. Our results reflect the strong and immediate positive effect of changes in human activities on air quality and the atmospheric role of BC aerosols as a major air pollutant in the Anthropocene. [ABSTRACT FROM AUTHOR]

We used the objective analysis method in conjunction with the successive correction method to assimilate MODerate resolution Imaging Spectroradiometer (MODIS) Aerosol Optical Depth (AOD) data into the Chimère model in order to improve the modeling of fine particulate matter (PM 2.5 ) concentrations and AOD field over Europe. A data assimilation module was developed to adjust the daily initial total column aerosol concentrations based on a forecast-analysis cycling scheme. The model is then evaluated during one-month winter period to examine how such a data assimilation technique pushes the model results closer to surface observations. This comparison showed that the mean biases of both surface PM 2.5 concentrations and the AOD field could be reduced from − 34 to −15% and from −45 to −27%. The assimilation, however, leads to false alarms because of the difficulty in distributing AOD 550 over different particle sizes. The impact of the influence radius is found to be small and depends on the density of satellite data. This work, although preliminary, is important in terms of near-real time air quality forecasting using the Chimère model and can be further developed to improve modeled PM 2.5 and ozone concentrations. [ABSTRACT FROM AUTHOR]

Aerosols play a crucial role in climate through different feedback mechanisms, affecting radiation, clouds, and air column stability. This study focuses on the altitude dependence of the cloud-mediated indirect effects of aerosols in the Great Alpine Region (GAR), an area characterized by high pollution levels from anthropic activities in the Po Valley and a complex orography with some of the highest mountains in Europe. Using a regional atmospheric model, 5-year-long convective-permitting sensitivity experiments have been run with different surface aerosol fluxes. The results show that seasonal mean cloud cover, temperature, and precipitations are affected by the aerosol concentrations in the air column and that the response to pollution is both elevation- and season-dependent. The overall cloud cover increase with aerosol levels leads to either surface cooling or warming depending on the surface albedo (snow covered or not). Furthermore, different types of clouds have a different response: while the lifetime of low-pressure-system clouds and orographic clouds is generally increased at high levels of aerosols, convective clouds (typical of the summer season) can decrease at high levels of pollution due to the reduction in strong updrafts associated with an increased air column stability. [ABSTRACT FROM AUTHOR]

The predictability of deep moist convection is subject to large uncertainties resulting from inaccurate initial and boundary data, the incomplete description of physical processes, or microphysical uncertainties. In this study, we investigate the response of convective clouds and precipitation over central Europe to varying cloud condensation nuclei (CCN) concentrations and different shape parameters of the cloud droplet size distribution (CDSD), both of which are not well constrained by observations. We systematically evaluate the relative impact of these uncertainties in realistic convection-resolving simulations for multiple cases with different synoptic controls using the new icosahedral non-hydrostatic ICON model. The results show a large systematic increase in total cloud water content with increasing CCN concentrations and narrower CDSDs, together with a reduction in the total rain water content. This is related to a suppressed warm-rain formation due to a less efficient collision–coalescence process. It is shown that the evaporation at lower levels is responsible for diminishing these impacts on surface precipitation, which lies between +13 % and -16 % compared to a reference run with continental aerosol assumption. In general, the precipitation response was larger for weakly forced cases. We also find that the overall timing of convection is not sensitive to the microphysical uncertainties applied, indicating that different rain intensities are responsible for changing precipitation totals at the ground. Furthermore, weaker rain intensities in the developing phase of convective clouds can allow for a higher convective instability at later times, which can lead to a turning point with larger rain intensities later on. The existence of such a turning point and its location in time can have a major impact on precipitation totals. In general, we find that an increase in the shape parameter can produce almost as large a variation in precipitation as a CCN increase from maritime to polluted conditions. The narrowing of the CDSD not only decreases the absolute values of autoconversion and accretion but also decreases the relative role of the warm-rain formation in general, independent of the prevailing weather regime. We further find that increasing CCN concentrations reduce the effective radius of cloud droplets in a stronger manner than larger shape parameters. The cloud optical depth, however, reveals a similarly large increase with larger shape parameters when changing the aerosol load from maritime to polluted. By the frequency of updrafts as a function of height, we show a negative aerosol effect on updraft strength, leading to an enervation of deep convection. These findings demonstrate that both the CCN assumptions and the CDSD shape parameter are important for quantitative precipitation forecasting and should be carefully chosen if double-moment schemes are used for modeling aerosol–cloud interactions. [ABSTRACT FROM AUTHOR]

PMCAMx-UF, a three-dimensional chemical transport model focusing on the simulation of the ultrafine particle size distribution and composition has been extended with the addition of reactions of chemical aging of semivolatile anthropogenic organic vapors, the emissions and chemical aging of intermediate-volatility organic compounds (IVOCs), and the production of extremely low-volatility organic compounds (ELVOCs) by monoterpenes. The model is applied in Europe to quantify the effect of these processes on particle number concentrations. The model predictions are evaluated against both ground measurements collected during the PEGASOS 2012 summer campaign across many stations in Europe and airborne observations by a zeppelin measuring above Po Valley, Italy. PMCAMx-UF reproduces the ground level daily average concentrations of particles with a diameter larger than 100 nm (N100) with normalized mean error (NME) of 45 % and normalized mean bias (NMB) close to 10 %. For the same simulation, PMCAMx-UF tends to overestimate the concentration of particles with a diameter larger than 10 nm (N10) with a daily NMB of 23 % and a daily NME of 63 %. The model was able to reproduce more than 75 % of the N10 and N100 airborne observations (zeppelin) within a factor of 2. According to the PMCAMx-UF predictions, the ELVOC production by monoterpenes leads to surprisingly small changes of the average number concentrations over Europe. The total number concentration decreased due to the ELVOC formation by 0.2 %, N10 decreased by 1.1 %, N50 (particles with a diameter larger than 50 nm) increased by 3 %, and N100 increased by 4 % due to this new secondary organic aerosol (SOA) source. This small change is due to the nonlinearity of the system, with increases predicted in some areas and decreases in others, but also the cancelation of the effects of the various processes like accelerated growth and accelerated coagulation. Locally, the effects can be significant. For example, an increase in N100 by 20 %–50 % is predicted over Scandinavia and significant increases (10 %–20 %) are predicted over some parts of central Europe. The ELVOCs contributed on average around 0.5 µgm-3 and accounted for 10 %–15 % of the PM2.5 OA. The addition of IVOC emissions and their aging reactions led to a surprising reduction of the total number of particles (Ntot) and N10 by 10 %–15 % and 5 %–10 %, respectively, and to an increase in the concentration of N100 by 5 %–10 %. These were due to the accelerated coagulation and reduced nucleation rates. [ABSTRACT FROM AUTHOR]

Secondary inorganic PM 2.5 particles are formed from SOx (SO2+SO42-), NOx (NO+NO2), and NH3 emissions, through the formation of either ammonium sulfate ((NH4)2SO4) or ammonium nitrate (NH4NO3). EU limits and WHO guidelines for PM 2.5 levels are frequently exceeded in Europe, in particular in the winter months. In addition the critical loads for eutrophication are exceeded in most of the European continent. Further reductions in NH3 emissions and other PM precursors beyond the 2030 requirements could alleviate some of the health burden from fine particles and also reduce the deposition of nitrogen to vulnerable ecosystems. Using the regional-scale EMEP/MSC-W model, we have studied the effects of year 2030 NH3 emissions on PM 2.5 concentrations and depositions of nitrogen in Europe in light of present (2017), past (2005), and future (2030) conditions. Our calculations show that in Europe the formation of PM 2.5 from NH3 to a large extent is limited by the ratio between the emissions of NH3 on one hand and SOx plus NOx on the other hand. As the ratio of NH3 to SOx and NOx is increasing, the potential to further curb PM 2.5 levels through reductions in NH3 emissions is decreasing. Here we show that per gram of NH3 emissions mitigated, the resulting reductions in PM 2.5 levels simulated using 2030 emissions are about a factor of 2.6 lower than when 2005 emissions are used. However, this ratio is lower in winter. Thus further reductions in the NH3 emissions in winter may have similar potential to SOx and NOx in curbing PM 2.5 levels in this season. Following the expected reductions of NH3 emission, depositions of reduced nitrogen (NH3+NH4+) should also decrease in Europe. However, as the reductions in NOx emission are larger than for NH3 , the fraction of total nitrogen (reduced plus oxidised nitrogen) deposited as reduced nitrogen is increasing and may exceed 60 % in most of Europe by 2030. Thus the potential for future reductions in the exceedances of critical loads for eutrophication in Europe will mainly rely on the ability to reduce NH3 emissions. [ABSTRACT FROM AUTHOR]

The variability of the westerly jet stream and storm track is crucial for summer weather and climate in the North Atlantic/European region. Observations for recent decades show notable trends in the summer jet from the 1970s to 2010s, characterized by an equatorward migration over the North Atlantic accompanied by a poleward migration and weakening of the Mediterranean jet over Europe. These changes in atmospheric circulation were associated with more cyclonic storms traveling across the United Kingdom into northern Europe, and fewer over the Mediterranean, leading to wet summers in northern Europe and dry summers in southern Europe. In this study we investigate the potential drivers and processes that may have been responsible for the observed changes in summer atmospheric circulation, with a particular focus on the role of anthropogenic aerosols (AA). We conduct attribution experiments with an atmospheric general circulation model (AGCM) forced with observed changes in sea surface temperatures/sea ice extent (SST/SIE), greenhouse gas concentrations, and AA precursor emissions. Comparison between the model results and observations strongly suggests that fast responses to AA changes were likely the primary driver of the observed poleward migration and weakening of the Mediterranean jet, with changes in SST/SIE playing a secondary role. The simulated response shows good agreement with the observed changes in both magnitude and vertical structure, which suggests that common mechanisms, involving aerosol–radiation and aerosol–cloud interactions, are responsible. By contrast, changes in the North Atlantic jet are influenced in the model experiments by changes in both Atlantic SST/SIE (which may themselves have been influenced by changes in AA) and fast responses to AA. In this case, however, there are significant differences between the model response and the observed changes; we argue that these differences may be explained by biases in the model climatology. [ABSTRACT FROM AUTHOR]

This study investigates, through regional climate modelling, the surface mass concentration and AOD (aerosol optical depth) evolution of the various (anthropogenic and natural) aerosols over the Euro-Mediterranean region between the end of the 20th century and the mid-21st century. The direct aerosol radiative forcing (DRF) as well as the future Euro-Mediterranean climate sensitivity to aerosols have also been analysed. Different regional climate simulations were carried out with the CNRM-ALADIN63 regional climate model, driven by the global CNRM-ESM2-1 Earth system model (used in CMIP6) and coupled to the TACTIC (Tropospheric Aerosols for ClimaTe In CNRM) interactive aerosol scheme. These simulations follow several future scenarios called shared socioeconomic pathways (SSP 1-1.9, SSP 3-7.0 and SSP 5-8.5), which have been chosen to analyse a wide range of possible future scenarios in terms of aerosol or particle precursor emissions. Between the historical and the future period, results show a total AOD decrease between 30 % and 40 % over Europe for the three scenarios, mainly due to the sulfate AOD decrease (between -85 and -93 %), that is partly offset by the nitrate and ammonium particles AOD increase (between +90 and +120 %). According to these three scenarios, nitrate aerosols become the largest contributor to the total AOD during the future period over Europe, with a contribution between 43.5 % and 47.5 %. It is important to note that one of the precursors of nitrate and ammonium aerosols, nitric acid, has been implemented in the model as a constant climatology over time. Concerning natural aerosols, their contribution to the total AOD increases slightly between the two periods. The different evolution of aerosols therefore impacts their DRF, with a significant sulfate DRF decrease between 2.4 and 2.8 W m -2 and a moderate nitrate and ammonium DRF increase between 1.3 and 1.5 W m -2 , depending on the three scenarios over Europe. These changes, which are similar under the different scenarios, explain about 65 % of the annual shortwave radiation change but also about 6 % (in annual average) of the warming expected over Europe by the middle of the century. This study shows, with SSP 5-8.5, that the extra warming attributable to the anthropogenic aerosol evolution over Central Europe and the Iberian Peninsula during the summer period is due to "aerosol–radiation" as well as "aerosol–cloud" interaction processes. The extra warming of about 0.2 ∘ C over Central Europe is explained by a surface radiation increase of 5.8 W m -2 over this region, due to both a surface aerosol DRF decrease of 4.4 W m -2 associated with a positive effective radiative forcing due to aerosol–radiation interactions (ERFari) of 2.7 W m -2 at the top of the atmosphere (TOA) and a cloud optical depth (COD) decrease of 1.3. In parallel, the simulated extra warming of 0.2 ∘ C observed over the Iberian Peninsula is due to a COD decrease of 1.3, leading to a positive effective radiative forcing due to aerosol–cloud interactions (ERFaci) of 2.6 W m -2 at the TOA but also to an atmospheric dynamics change leading to a cloud cover decrease of about 1.7 % and drier air in the lower layers, which is a signature of the semi-direct forcing. This study thus highlights the necessity of taking into account the evolution of aerosols in future regional climate simulations. [ABSTRACT FROM AUTHOR]

Increasing evidence from experimental studies suggests that the losses of semi-volatile vapors to chamber walls could be responsible for the underestimation of organic aerosol (OA) in air quality models that use parameters obtained from chamber experiments. In this study, a box model with a volatility basis set (VBS) scheme was developed, and the secondary organic aerosol (SOA) yields with vapor wall loss correction were optimized by a genetic algorithm based on advanced chamber experimental data for biomass burning. The vapor wall loss correction increases the SOA yields by a factor of 1.9–4.9 and leads to better agreement with measured OA for 14 chamber experiments under different temperatures and emission loads. To investigate the influence of vapor wall loss correction on regional OA simulations, the optimized parameterizations (SOA yields, emissions of intermediate-volatility organic compounds from biomass burning, and enthalpy of vaporization) were implemented in the regional air quality model CAMx (Comprehensive Air Quality Model with extensions). The model results from the VBS schemes with standard (VBS_BASE) and vapor-wall-loss-corrected parameters (VBS_WLS), as well as the traditional two-product approach, were compared and evaluated by OA measurements from five Aerodyne aerosol chemical speciation monitor (ACSM) or aerosol mass spectrometer (AMS) stations in the winter of 2011. An additional reference scenario, VBS_noWLS, was also developed using the same parameterization as VBS_WLS except for the SOA yields, which were optimized by assuming there is no vapor wall loss. The VBS_WLS generally shows the best performance for predicting OA among all OA schemes and reduces the mean fractional bias from -72.9 % (VBS_BASE) to -1.6 % for the winter OA. In Europe, the VBS_WLS produces the highest domain average OA in winter (2.3 µgm-3), which is 106.6 % and 26.2 % higher than VBS_BASE and VBS_noWLS, respectively. Compared to VBS_noWLS, VBS_WLS leads to an increase in SOA by up to ∼80 % (in the Balkans). VBS_WLS also leads to better agreement between the modeled SOA fraction in OA (fSOA) and the estimated values in the literature. The substantial influence of vapor wall loss correction on modeled OA in Europe highlights the importance of further improvements in parameterizations based on laboratory studies for a wider range of chamber conditions and field observations with higher spatial and temporal coverage. [ABSTRACT FROM AUTHOR]

The amount of solar radiation reaching the Earth's surface can be highly determined by atmospheric aerosols, which have been pointed to as the most uncertain climate forcing agents through their direct (scattering and absorption), semi-direct (absorption implying a thermodynamic effect on clouds) and indirect (modification of cloud properties when aerosols act as cloud condensation nuclei) effects. Nonetheless, regional climate models hardly ever dynamically model the atmospheric concentration of aerosols and their interactions with radiation (ARIs) and clouds (ACIs). The objective of this work is to evince the role of modeling ARIs and ACIs in Weather Research and Forecast (WRF) model simulations with fully interactive aerosols (online resolved concentrations) with a focus on summer mean surface downward solar radiation (RSDS) over Europe. Under historical conditions (1991–2010), both ARIs and ACIs reduce RSDS by a few percentage points over central and northern regions. This reduction is larger when only ARIs are resolved, while ACIs counteract the effect of the former by up to half. The response of RSDS to the activation of ARIs and ACIs is mainly led by the aerosol effect on cloud coverage, while the aerosol effect on atmospheric optical depth plays a very minor role, which evinces the importance of semi-direct and indirect aerosol effects. In fact, differences in RSDS among experiments with and without aerosols are smaller under clear-sky conditions. In terms of future projections (2031–2050 vs. 1991–2010), the baseline pattern (from an experiment without aerosols) shows positive signals southward and negative signals northward. While ARIs enhance the former and reduce the latter, ACIs work in the opposite direction and provide a flatter RSDS change pattern, further evincing the opposite impact from semi-direct and indirect effects and the nontrivial influence of the latter. [ABSTRACT FROM AUTHOR]

The dependence of aerosol acidity on particle size, location, and altitude over Europe during a summertime period is investigated using the hybrid version of aerosol dynamics in the chemical transport model PMCAMx. The pH changes more with particle size in northern and southern Europe owing to the enhanced presence of non-volatile cations (Na, Ca, K, Mg) in the larger particles. Differences of up to 1–4 pH units are predicted between sub- and supermicron particles, while the average pH of PM1-2.5 can be as much as 1 unit higher than that of PM1. Most aerosol water over continental Europe is associated with PM1 , while coarse particles dominate the water content in the marine and coastal areas due to the relatively higher levels of hygroscopic sea salt. Particles of all sizes become increasingly acidic with altitude (0.5–2.5 units pH decrease over 2.5 km) primarily because of the decrease in aerosol liquid water content (driven by humidity changes) with height. Inorganic nitrate is strongly affected by aerosol pH with the highest average nitrate levels predicted for the PM1-5 range and over locations where the pH exceeds 3. Dust tends to increase aerosol pH for all particle sizes and nitrate concentrations for supermicron range particles. This effect of dust is quite sensitive to its calcium content. The size-dependent pH differences carry important implications for pH-sensitive processes in the aerosol. [ABSTRACT FROM AUTHOR]

The effect of aerosols on regional climate simulations presents large uncertainties due to their complex and non-linear interactions with a wide variety of factors, including aerosol–radiation (ARI) and aerosol–cloud (ACI) interactions. These interactions are strongly conditioned by the meteorological situation and type of aerosol, but, despite their increase, only a limited number of studies have covered this topic from a regional and climatic perspective. This contribution thus aims to quantify the impacts on precipitation of the inclusion of ARI and ACI processes in regional climate simulations driven by ERA20C reanalysis. A series of regional climatic simulations (for the period 1991–2010) for the Euro-CORDEX domain were conducted including ARI and ARI + ACI (ARCI), establishing as a reference a simulation where aerosols were not included interactively (BASE). The results show that the effects of ARI and ACI on time-mean spatially averaged precipitation over the whole domain are limited. However, a spatial redistribution of precipitation occurs when the ARI and ACI processes are introduced into the model, as well do changes in the precipitation intensity regimes. The main differences with respect to the base-case simulations occur in central Europe, where a decrease in precipitation is associated with a depletion in the number of rainy days and clouds at low level (CLL). This reduction in precipitation presents a strong correlation with the ratio PM 2.5/ PM 10 , since the decrease is especially intense during those events with high values of that ratio (pointing to high levels of anthropogenic aerosols) over central Europe. The precipitation decrease occurs for all ranges of precipitation rates. On the other hand, the model produces an increase in precipitation over the eastern Mediterranean basin associated with an increase in clouds and rainy days when ACIs are implemented. Here, the change is caused by the high presence of PM 10 (low PM 2.5/ PM 10 ratios, pointing to natural aerosols). In this case, the higher amount of precipitation affects only days with low rates of precipitation. Finally, there are some disperse areas where the inclusion of aerosols leads to an increase in precipitation, especially for moderate and high precipitation rates. [ABSTRACT FROM AUTHOR]

The size distribution of atmospheric aerosols plays a key role for understanding and quantifying the uncertainties related to aerosol–radiation and aerosol–cloud interactions. These interactions ultimately depend on the size distribution through optical properties (such as aerosol optical depth, AOD) or cloud microphysical properties. Hence, the main objective of this contribution is to disentangle the impact of the representation of aerosol size distribution on aerosol optical properties over central Europe, particularly over the Mediterranean Basin, during a summertime aerosol episode. To fulfill this objective, a sensitivity test has been conducted using the coupled chemistry–meteorology model WRF-Chem (Weather Research Forecast model coupled with Chemistry). The test modified the parameters defining a lognormal size distribution (geometric diameter and standard deviation) by 10 %, 20 %, and 50 %. Results reveal that the reduction in the standard deviation of the accumulation mode leads to the largest impacts on AOD due to a transfer of particles from the accumulation mode to the coarse mode. A reduction in the geometric diameter of the accumulation mode also has an influence on AOD representation since particles in this mode are assumed to be smaller. In addition, an increase in the geometric diameter of the coarse mode produces a redistribution through the total size distribution by relocating particles from the finer modes to the coarse. [ABSTRACT FROM AUTHOR]

We examine the capability of near-spherical-shaped particles to reproduce the triple-wavelength particle linear depolarization ratio (PLDR) and lidar ratio (LR) values measured over Europe for stratospheric smoke originating from Canadian wildfires. The smoke layers were detected both in the troposphere and the stratosphere, though in the latter case the particles presented PLDR values of almost 18 % at 532 nm as well as a strong spectral dependence from the UV to the near-IR wavelength. Although recent simulation studies of rather complicated smoke particle morphologies have shown that heavily coated smoke aggregates can produce large PLDR, herein we propose a much simpler model of compact near-spherical smoke particles. This assumption allows for the reproduction of the observed intensive optical properties of stratospheric smoke, as well as their spectral dependence. We further examine whether an extension of the current Aerosol Robotic Network (AERONET) scattering model to include the near-spherical shapes could be of benefit to the AERONET retrieval for stratospheric smoke cases associated with enhanced PLDR. Results of our study illustrate the fact that triple-wavelength PLDR and LR lidar measurements can provide us with additional insight when it comes to particle characterization. [ABSTRACT FROM AUTHOR]

In mid-October 2017 Storm Ophelia crossed over western coastal Europe, inducing the combined transport of Saharan dust and Iberian biomass burning aerosols over several European areas. In this study we assess the performance of the Copernicus Atmosphere Monitoring Service (CAMS) forecast systems during this complex aerosol transport event and the potential benefits that data assimilation and regional models could bring. To this end, CAMS global and regional forecast data are analysed and compared against observations from passive (MODIS: Moderate Resolution Imaging Spectroradiometer aboard Terra and Aqua) and active (CALIOP/CALIPSO: Cloud-Aerosol LIdar with Orthogonal Polarization aboard Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations) satellite sensors and ground-based measurements (EMEP: European Monitoring and Evaluation Programme). The analysis of the CAMS global forecast indicates that dust and smoke aerosols, discretely located on the warm and cold fronts of Ophelia, respectively, were affecting the aerosol atmospheric composition over Europe during the passage of the Storm. The observed MODIS aerosol optical depth (AOD) values are satisfactorily reproduced by the CAMS global forecast system, with a correlation coefficient of 0.77 and a fractional gross error (FGE) of 0.4. The comparison with a CAMS global control simulation not including data assimilation indicates a significant improvement in the bias due to data assimilation implementation, as the FGE decreases by 32 %. The qualitative evaluation of the IFS (Integrated Forecast System) dominant-aerosol type and location against the CALIPSO observations overall reveals a good agreement. Regarding the footprint on air quality, both CAMS global and regional forecast systems are generally able to reproduce the observed signal of increase in surface particulate matter concentrations. The regional component performs better in terms of bias and temporal variability, with the correlation deteriorating over forecast time. Yet, both products exhibit inconsistencies on the quantitative and temporal representation of the observed surface particulate matter enhancements, stressing the need for further development of the air quality forecast systems for even more accurate and timely support of citizens and policy-makers. [ABSTRACT FROM AUTHOR]

The aerosol mass spectrometer (AMS), combined with statistical methods such as positive matrix factorization (PMF), has greatly advanced the quantification of primary organic aerosol (POA) sources and total secondary organic aerosol (SOA) mass. However, the use of thermal vaporization and electron ionization yields extensive thermal decomposition and ionization-induced fragmentation, which limit chemical information needed for SOA source apportionment. The recently developed extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF) provides mass spectra of the organic aerosol fraction with a linear response to mass and no thermal decomposition or ionization-induced fragmentation. However, the costs and operational requirements of online instruments make their use impractical for long-term or spatially dense monitoring applications. This challenge was overcome for AMS measurements by measuring re-nebulized water extracts from ambient filter samples. Here, we apply the same strategy for EESI-TOF measurements of 1 year of 24 h filter samples collected approximately every fourth day throughout 2013 at an urban site. The nebulized water extracts were measured simultaneously with an AMS. The application of positive matrix factorization (PMF) to EESI-TOF spectra resolved seven factors, which describe water-soluble OA: less and more aged biomass burning aerosol (LABB EESI and MABB EESI , respectively), cigarette-smoke-related organic aerosol, primary biological organic aerosol, biogenic secondary organic aerosol, and a summer mixed oxygenated organic aerosol factor. Seasonal trends and relative contributions of the EESI-TOF OA sources were compared with AMS source apportionment factors, measured water-soluble ions, cellulose, and meteorological data. Cluster analysis was utilized to identify key factor-specific ions based on PMF. Both LABB and MABB contribute strongly during winter. LABB is distinguished by very high signals from C6H10O5 (levoglucosan and isomers) and C8H12O6 , whereas MABB is characterized by a large number of CxHyOz and CxHyOzN species of two distinct populations: one with low H:C and high O:C and the other with high H:C and low O:C. Two oxygenated summertime SOA sources were attributed to terpene-derived biogenic SOA, a major summertime aerosol source in central Europe. Furthermore, a primary biological organic aerosol factor was identified, which was dominated by plant-derived fatty acids and correlated with free cellulose. The cigarette-smoke-related factor contained a high contribution of nicotine and high abundance of organic nitrate ions with low m/z. [ABSTRACT FROM AUTHOR]

A novel method has been developed to estimate aerosol optical depth (AOD) from sunshine duration (SD) measurements under cloud-free conditions. It is a physically based method serving for the reconstruction of the historical evolution of AOD during the last century. In addition to sunshine duration data, it requires daily water vapor and ozone products as inputs taken from the ECMWF 20th century reanalysis ERA-20C, available at the global scale over the period 1900–2010. Surface synoptic cloud observations are used to identify cloud-free days. For 16 sites over Europe, the accuracy of the estimated daily AOD, and its seasonal variability, is similar to or better than those from two earlier methods when compared to AErosol RObotic NETwork measurements. In addition, it also improves the detection of the signal from massive aerosol events such as important volcanic eruptions (e.g., Arenal and Fernandina Island in 1968, El Chichón in 1982 and Pinatubo in 1992). Finally, the reconstructed AOD time series are in good agreement with the dimming/brightening phenomenon and also provide preliminary evidence of the early-brightening phenomenon. [ABSTRACT FROM AUTHOR]

In this work we present downscaling experiments with the Weather Research and Forecasting model (WRF) to test the sensitivity to resolving aerosol–radiation and aerosol–cloud interactions on simulated regional climate for the EURO-CORDEX domain. The sensitivities mainly focus on the aerosol–radiation interactions (direct and semi-direct effects) with four different aerosol optical depth datasets (Tegen, MAC-v1, MACC, GOCART) being used and changes to the aerosol absorptivity (single scattering albedo) being examined. Moreover, part of the sensitivities also investigates aerosol–cloud interactions (indirect effect). Simulations have a resolution of 0.44 ∘ and are forced by the ERA-Interim reanalysis. A basic evaluation is performed in the context of seasonal-mean comparisons to ground-based (E-OBS) and satellite-based (CM SAF SARAH, CLARA) benchmark observational datasets. The impact of aerosols is calculated by comparing it against a simulation that has no aerosol effects. The implementation of aerosol–radiation interactions reduces the direct component of the incoming surface solar radiation by 20 %–30 % in all seasons, due to enhanced aerosol scattering and absorption. Moreover the aerosol–radiation interactions increase the diffuse component of surface solar radiation in both summer (30 %–40 %) and winter (5 %–8 %), whereas the overall downward solar radiation at the surface is attenuated by 3 %–8 %. The resulting aerosol radiative effect is negative and is comprised of the net effect from the combination of the highly negative direct aerosol effect (-17 to -5 W m -2) and the small positive changes in the cloud radiative effect (+5 W m -2), attributed to the semi-direct effect. The aerosol radiative effect is also stronger in summer (-12 W m -2) than in winter (-2 W m -2). We also show that modelling aerosol–radiation and aerosol–cloud interactions can lead to small changes in cloudiness, mainly regarding low-level clouds, and circulation anomalies in the lower and mid-troposphere, which in some cases, mainly close to the Black Sea in autumn, can be of statistical significance. Precipitation is not affected in a consistent pattern throughout the year by the aerosol implementation, and changes do not exceed ± 5 % except for the case of unrealistically absorbing aerosol. Temperature, on the other hand, systematically decreases by -0.1 to -0.5 ∘ C due to aerosol–radiation interactions with regional changes that can be up to -1.5 ∘ C. [ABSTRACT FROM AUTHOR]

Aerosols may impact precipitation in a complex way involving their direct and indirect effects. In a previous numerical study, the overall microphysical effect of aerosols was found to weaken precipitation through reduced precipitable water and convective instability. The present study aims to quantify the relative importance of these two processes in the reduction of summer precipitation using temperature–precipitation scaling. Based on a numerical sensitivity experiment conducted in central Europe aiming to isolate indirect effects, the results show that, all others effects being equal, the scaling of hourly convective precipitation with temperature follows the Clausius–Clapeyron (CC) relationship, whereas the decrease in convective precipitation does not scale with the CC law since it is mostly attributable to increased stability with increased aerosol concentration rather than to decreased precipitable water content. This effect is larger at low surface temperatures at which clouds are statistically more frequent and optically thicker. At these temperatures, the increase in stability is mostly linked to the stronger reduction in temperature in the lower troposphere compared to the upper troposphere, which results in lower lapse rates. [ABSTRACT FROM AUTHOR]

The VBS-GECKO (volatility basis set – Generator for Explicit Chemistry and Kinetics of Organics in the Atmosphere) parameterization for secondary organic aerosol (SOA) formation was integrated into the chemistry-transport model CHIMERE. Concentrations of organic aerosol (OA) and SOA were simulated over Europe for the July–August 2013 period. Simulated concentrations with VBS-GECKO were compared to results obtained with the former H2O parameterization implemented in CHIMERE and to observations from EMEP, ACTRIS and other observations available in the EBAS database. The model configuration using the VBS-GECKO parameterization slightly improves the performances compared to the model configuration using the former H2O parameterization. The VBS-GECKO model configuration performs well for stations showing a large SOA concentration from biogenic sources, especially in northern Europe, but underestimates OA concentrations over stations close to urban areas. Simulated OA was found to be mainly secondary (∼85 %) and from terpene oxidation. Simulations show negligible contribution of the oxidation of mono-aromatic compounds to SOA production. Tests performed to examine the sensitivity of simulated OA concentrations to hydro-solubility, volatility, aging rates and NOx regime have shown that the VBS-GECKO parameterization provides consistent results, with a weak sensitivity to changes in the parameters provided by the gas-phase mechanism included in CHIMERE (e.g., HOx or NOx concentrations). Different scenarios considering intermediate-volatility organic compound (IVOC) emissions were tested to examine the contribution of IVOC oxidation to SOA production. At the continental scale, these simulations show a weak sensitivity of OA concentrations to IVOC emission variations. At the local scale, accounting for IVOC emissions was found to lead to a substantial increase in OA concentrations in the plume from urban areas. This additional OA source remains too small to explain the gap between simulated and measured values at stations where anthropogenic sources are dominant. [ABSTRACT FROM AUTHOR]

Aerosols have significantly affected health, environment, and climate in Europe. Aerosol concentrations have been declining since the 1980s in Europe, mainly owing to a reduction of local aerosol and precursor emissions. Emissions from other source regions of the world, which have been changing rapidly as well, may also perturb the historical and future trends of aerosols and change their radiative impact in Europe. This study examines trends of aerosols in Europe during 1980–2018 and quantifies contributions from 16 source regions using the Community Atmosphere Model version 5 with Explicit Aerosol Source Tagging (CAM5-EAST). The simulated near-surface total mass concentration of sulfate, black carbon, and primary organic carbon had a 62 % decrease during 1980–2018. The majority of which was contributed to reductions of local emissions in Europe, and 8 %–9 % was induced by a decrease in emissions from Russia–Belarus–Ukraine. With the decreases in the fractional contribution of local emissions, aerosols transported from other source regions are increasingly important for air quality in Europe. During 1980–2018, the decrease in sulfate loading led to a warming effect of 2.0 W m -2 in Europe, with 12 % coming from changes in non-European sources, especially from North America and Russia–Belarus–Ukraine. According to the Shared Socioeconomic Pathways (SSP) scenarios, contributions to the sulfate radiative forcing over Europe from both local European emissions and non-European emissions should decrease at a comparable rate in the next 3 decades, suggesting that future changes in non-European emissions are as important as European emissions for causing possible regional climate change associated with aerosols in Europe. [ABSTRACT FROM AUTHOR]

Source apportionment of organic aerosols (OAs) is of great importance to better understand the health impact and climate effects of particulate matter air pollution. Air quality models are used as potential tools to identify OA components and sources at high spatial and temporal resolution; however, they generally underestimate OA concentrations, and comparisons of their outputs with an extended set of measurements are still rare due to the lack of long-term experimental data. In this study, we addressed such challenges at the European level. Using the regional Comprehensive Air Quality Model with Extensions (CAMx) and a volatility basis set (VBS) scheme which was optimized based on recent chamber experiments with wood burning and diesel vehicle emissions, and which contains more source-specific sets compared to previous studies, we calculated the contribution of OA components and defined their sources over a whole-year period (2011). We modeled separately the primary and secondary OA contributions from old and new diesel and gasoline vehicles, biomass burning (mostly residential wood burning and agricultural waste burning excluding wildfires), other anthropogenic sources (mainly shipping, industry and energy production) and biogenic sources. An important feature of this study is that we evaluated the model results with measurements over a longer period than in previous studies, which strengthens our confidence in our modeled source apportionment results. Comparison against positive matrix factorization (PMF) analyses of aerosol mass spectrometric measurements at nine European sites suggested that the modified VBS scheme improved the model performance for total OA as well as the OA components, including hydrocarbon-like (HOA), biomass burning (BBOA) and oxygenated components (OOA). By using the modified VBS scheme, the mean bias of OOA was reduced from -1.3 to -0.4 µ g m -3 corresponding to a reduction of mean fractional bias from -45 % to -20 %. The winter OOA simulation, which was largely underestimated in previous studies, was improved by 29 % to 42 % among the evaluated sites compared to the default parameterization. Wood burning was the dominant OA source in winter (61 %), while biogenic emissions contributed ∼ 55 % to OA during summer in Europe on average. In both seasons, other anthropogenic sources comprised the second largest component (9 % in winter and 19 % in summer as domain average), while the average contributions of diesel and gasoline vehicles were rather small (∼ 5 %) except for the metropolitan areas where the highest contribution reached 31 %. The results indicate the need to improve the emission inventory to include currently missing and highly uncertain local emissions, as well as further improvement of VBS parameterization for winter biomass burning. Although this study focused on Europe, it can be applied in any other part of the globe. This study highlights the ability of long-term measurements and source apportionment modeling to validate and improve emission inventories, and identify sources not yet properly included in existing inventories. [ABSTRACT FROM AUTHOR]

Size-resolved aerosol trends were investigated based on a 17-year data set (2000–2017) from the rural background site Aspvreten located in southern Sweden (58.8 ∘ N, 17.4 ∘ E). Cluster analysis of the size distributions was performed to aid in the interpretation of the data. The results confirm previous findings of decreasing aerosol mass and number during the last decades as a result of reduced anthropogenic emissions in Europe. We show that both particle modal number concentration and size have substantially been reduced during the last 17 years. Negative trends in particle number concentration of about 10 cm -3 yr -1 are present for nuclei, Aitken, and accumulation modes. In total, integral particle number concentration has decreased by 30 %, from 1860 to ca. 1300 cm -3. The reduction in modal number concentration is accompanied by a decrease in modal size, and this decrease is largest for the accumulation mode (2 nm yr -1 or about 17 % for the whole period). These reductions have resulted in a decrease in submicron particle mass (< 390 nm) by more than 50 % over the period 2000–2017. These decreases are similar to observations found at other stations in northern Europe. Although all size classes show a downward trend as annual averages, we also show that observed trends are not evenly distributed over the year and that a rather complex picture emerges where both sign and magnitude of trends vary with season and size. The strongest negative trends are present during spring (accumulation mode) and autumn (Aitken mode). The strongest positive trends are present during summer months (Aitken mode). The combined trajectory and data analyses do not present evidence for an increase in new particle formation formed locally, although some evidence of increased new particle formation some distance away from the receptor is present. Observed aerosol size distribution data, together with an adiabatic cloud parcel model, were further used to estimate the change in cloud droplet concentration for various assumptions of updraught velocities and aerosol chemical composition. The results indicate a substantial increase in the atmospheric brightening effect due to a reduction in cloud reflectivity corresponding to 10 %–12 % reduction in cloud albedo over the period 2000–2017. [ABSTRACT FROM AUTHOR]

In the framework of the EURODELTA-Trends (EDT) modeling experiment, several chemical transport models (CTMs) were applied for the 1990–2010 period to investigate air quality changes in Europe as well as the capability of the models to reproduce observed long-term air quality trends. Five CTMs have provided modeled air quality data for 21 continuous years in Europe using emission scenarios prepared by the International Institute for Applied Systems Analysis/Greenhouse Gas – Air Pollution Interactions and Synergies (IIASA/GAINS) and corresponding year-by-year meteorology derived from ERA-Interim global reanalysis. For this study, long-term observations of particle sulfate (SO42-), total nitrate (TNO3), total ammonium (TNHx) as well as sulfur dioxide (SO2) and nitrogen dioxide (NO2) for multiple sites in Europe were used to evaluate the model results. The trend analysis was performed for the full 21 years (referred to as PT) but also for two 11-year subperiods: 1990–2000 (referred to as P1) and 2000–2010 (referred to as P2). The experiment revealed that the models were able to reproduce the faster decline in observed SO2 concentrations during the first decade, i.e., 1990–2000, with a 64 %–76 % mean relative reduction in SO2 concentrations indicated by the EDT experiment (range of all the models) versus an 82 % mean relative reduction in observed concentrations. During the second decade (P2), the models estimated a mean relative reduction in SO2 concentrations of about 34 %–54 %, which was also in line with that observed (47 %). Comparisons of observed and modeled NO2 trends revealed a mean relative decrease of 25 % and between 19 % and 23 % (range of all the models) during the P1 period, and 12 % and between 22 % and 26 % (range of all the models) during the P2 period, respectively. Comparisons of observed and modeled trends in SO42- concentrations during the P1 period indicated that the models were able to reproduce the observed trends at most of the sites, with a 42 %–54 % mean relative reduction indicated by the EDT experiment (range of all models) versus a 57 % mean relative reduction in observed concentrations and with good performance also during the P2 and PT periods, even though all the models overpredicted the number of statistically significant decreasing trends during the P2 period. Moreover, especially during the P1 period, both modeled and observational data indicated smaller reductions in SO42- concentrations compared with their gas-phase precursor (i.e., SO2), which could be mainly attributed to increased oxidant levels and pH-dependent cloud chemistry. An analysis of the trends in TNO3 concentrations indicated a 28 %–39 % and 29 % mean relative reduction in TNO3 concentrations for the full period for model data (range of all the models) and observations, respectively. Further analysis of the trends in modeled HNO3 and particle nitrate (NO3-) concentrations revealed that the relative reduction in HNO3 was larger than that for NO3- during the P1 period, which was mainly attributed to an increased availability of "free ammonia". By contrast, trends in modeled HNO3 and NO3- concentrations were more comparable during the P2 period. Also, trends of TNHx concentrations were, in general, underpredicted by all models, with worse performance for the P1 period than for P2. Trends in modeled anthropogenic and biogenic secondary organic aerosol (ASOA and BSOA) concentrations together with the trends in available emissions of biogenic volatile organic compounds (BVOCs) were also investigated. A strong decrease in ASOA was indicated by all the models, following the reduction in anthropogenic non-methane VOC (NMVOC) precursors. Biogenic emission data provided by the modeling teams indicated a few areas with statistically significant increase in isoprene emissions and monoterpene emissions during the 1990–2010 period over Fennoscandia and eastern European regions (i.e., around 14 %–27 %), which was mainly attributed to the increase of surface temperature. However, the modeled BSOA concentrations did not linearly follow the increase in biogenic emissions. Finally, a comprehensive evaluation against positive matrix factorization (PMF) data, available during the second period (P2) at various European sites, revealed a systematic underestimation of the modeled SOA fractions of a factor of 3 to 11, on average, most likely because of missing SOA precursors and formation pathways, with reduced biases for the models that accounted for chemical aging of semi-volatile SOA components in the atmosphere. [ABSTRACT FROM AUTHOR]

We use the best currently available in situ and satellite-derived surface and top-of-the-atmosphere (TOA) shortwave radiation observations to explore climatological annual cycles of fractional (i.e., normalized by incoming radiation at the TOA) atmospheric shortwave absorption a ˜ on a global scale. The analysis reveals that a ˜ is a rather regional feature where the reported nonexisting a ˜ in Europe is an exception rather than the rule. In several regions, large and distinctively different a ˜ are apparent. The magnitudes of a ˜ reach values up to 10% in some regions, which is substantial given that the long-term global mean atmospheric shortwave absorption is roughly 23%. Water vapor and aerosols are identified as major drivers for a ˜ while clouds seem to play only a minor role for a ˜ . Regions with large annual cycles in aerosol emissions from biomass burning also show the largest a ˜ . As biomass burning is generally related to human activities, a ˜ is likely also anthropogenically intensified or forced in the respective regions. We also test if climate models are able to simulate the observed pattern of a ˜ . In regions where a ˜ is driven by the annual cycle of natural aerosols or water vapor, the models perform well. In regions with large a ˜ induced by biomass-burning aerosols, the models' performance is very limited. [ABSTRACT FROM AUTHOR]

Monitoring of aerosols and their temporal evolution is very important for climate and air quality studies. In this study, we present a climatology of aerosol optical and microphysical properties over a continental southeastern European area based on 9 years of observations from a Cimel sun-photometer operating at Magurele (Romania) in the framework of AErosol RObotic NETwork (AERONET). The site is characterized by high intra-annual and inter-annual variability of the total aerosol optical depth (AOD), which has two peaks, during March and August. For half year, from May to November, Magurele is affected by the transport of aerosols from the nearby city of Bucharest, since the dominant winds are from this direction. Thus, the predominant is the fine mode of aerosols. The high inter-annual and intra-annual variability of Angstrom exponent (440–870 nm) indicates the presence of aerosols of different sizes. Negative statistically significant trends at all AOD wavelengths, the order of 20–40% per decade, have been calculated for the 9-year period of study (2007–2016). These trends are mostly attributed to the reduction of the fine mode particles, showing that the implementation of the EU regulations for the decrease of particulate matter emissions in Bucharest has been beneficial. [ABSTRACT FROM AUTHOR]

The weather and climate conditions can provide favorable or unfavorable atmospheric background for the maintenance and development of haze events. This study investigates the potential impacts of Arctic warming on the variation of Northern Hemisphere mid-latitude aerosol optical depth (AOD) in winter when haze often occurs. We first analyze the spatio-temporal variability of wintertime AOD in mid-latitudes of Northern Hemisphere from NASA MERRA-2 for the period of 1980–2016 using the empirical orthogonal function analysis and morlet wavelet analysis. It showes increasing trend for AOD in East China and North India and decreasing trend for AOD in Europe and North America during last 37 years while inter-decadal fluctuations exist. In addition to the temporal trends of AOD, two long-term periodic variations with periods of about 7 and 11 years exist, which implies the potential impacts from natural variabilities. Further analysis shows high correlations between the mid-latitude winter AOD (WA) and Arctic summer (May and June) surface temperature (T56). Moreover, the Arctic summer surface temperature demonstrates similar periodic variations with periods of about 7–9 and 11–13 years. Both of these indicate the potential impacts of Arctic summer warming on mid-latitude winter pollution. We then analyze the temporal correlations between Arctic summer temperature and mid-latitude winter AOD in different regions. Arctic T56 correlates negatively with WA in Europe and North America, and positively with that in East Asia, North India and Middle East. Particularly, T56 in western sea of Novaya Zemlya has the most prominent correlation with the WA in mid-latitudes of East Asia, especially in East China. This implies that Arctic T56 in the Arctic circle of Europe could be used for rough estimates of winter AOD in East Asia. [ABSTRACT FROM AUTHOR]

A total of 16 global chemistry transport models and general circulation models have participated in this study; 14 models have been evaluated with regard to their ability to reproduce the near-surface observed number concentration of aerosol particles and cloud condensation nuclei (CCN), as well as derived cloud droplet number concentration (CDNC). Model results for the period 2011–2015 are compared with aerosol measurements (aerosol particle number, CCN and aerosol particle composition in the submicron fraction) from nine surface stations located in Europe and Japan. The evaluation focuses on the ability of models to simulate the average across time state in diverse environments and on the seasonal and short-term variability in the aerosol properties. There is no single model that systematically performs best across all environments represented by the observations. Models tend to underestimate the observed aerosol particle and CCN number concentrations, with average normalized mean bias (NMB) of all models and for all stations, where data are available, of -24 % and -35 % for particles with dry diameters >50 and >120 nm, as well as -36 % and -34 % for CCN at supersaturations of 0.2 % and 1.0 %, respectively. However, they seem to behave differently for particles activating at very low supersaturations (<0.1 %) than at higher ones. A total of 15 models have been used to produce ensemble annual median distributions of relevant parameters. The model diversity (defined as the ratio of standard deviation to mean) is up to about 3 for simulated N3 (number concentration of particles with dry diameters larger than 3 nm) and up to about 1 for simulated CCN in the extra-polar regions. A global mean reduction of a factor of about 2 is found in the model diversity for CCN at a supersaturation of 0.2 % (CCN 0.2) compared to that for N3 , maximizing over regions where new particle formation is important. An additional model has been used to investigate potential causes of model diversity in CCN and bias compared to the observations by performing a perturbed parameter ensemble (PPE) accounting for uncertainties in 26 aerosol-related model input parameters. This PPE suggests that biogenic secondary organic aerosol formation and the hygroscopic properties of the organic material are likely to be the major sources of CCN uncertainty in summer, with dry deposition and cloud processing being dominant in winter. Models capture the relative amplitude of the seasonal variability of the aerosol particle number concentration for all studied particle sizes with available observations (dry diameters larger than 50, 80 and 120 nm). The short-term persistence time (on the order of a few days) of CCN concentrations, which is a measure of aerosol dynamic behavior in the models, is underestimated on average by the models by 40 % during winter and 20 % in summer. In contrast to the large spread in simulated aerosol particle and CCN number concentrations, the CDNC derived from simulated CCN spectra is less diverse and in better agreement with CDNC estimates consistently derived from the observations (average NMB -13 % and -22 % for updraft velocities 0.3 and 0.6 m s -1 , respectively). In addition, simulated CDNC is in slightly better agreement with observationally derived values at lower than at higher updraft velocities (index of agreement 0.64 vs. 0.65). The reduced spread of CDNC compared to that of CCN is attributed to the sublinear response of CDNC to aerosol particle number variations and the negative correlation between the sensitivities of CDNC to aerosol particle number concentration (∂Nd/∂Na) and to updraft velocity (∂Nd/∂w). Overall, we find that while CCN is controlled by both aerosol particle number and composition, CDNC is sensitive to CCN at low and moderate CCN concentrations and to the updraft velocity when CCN levels are high. Discrepancies are found in sensitivities ∂Nd/∂Na and ∂Nd/∂w ; models may be predisposed to be too "aerosol sensitive" or "aerosol insensitive" in aerosol–cloud–climate interaction studies, even if they may capture average droplet numbers well. This is a subtle but profound finding that only the sensitivities can clearly reveal and may explain inter-model biases on the aerosol indirect effect. [ABSTRACT FROM AUTHOR]

Aerosol acidity plays a key role in secondary aerosol formation. The high-temporal-resolution PM 2.5 pH and size-resolved aerosol pH in Beijing were calculated with ISORROPIA II. In 2016–2017, the mean PM 2.5 pH (at relative humidity (RH) > 30 %) over four seasons was 4.5±0.7 (winter) > 4.4±1.2 (spring) > 4.3±0.8 (autumn) > 3.8±1.2 (summer), showing moderate acidity. In coarse-mode aerosols, Ca2+ played an important role in aerosol pH. Under heavily polluted conditions, more secondary ions accumulated in the coarse mode, leading to the acidity of the coarse-mode aerosols shifting from neutral to weakly acidic. Sensitivity tests also demonstrated the significant contribution of crustal ions to PM 2.5 pH. In the North China Plain (NCP), the common driving factors affecting PM 2.5 pH variation in all four seasons were SO42- , TNH3 (total ammonium (gas + aerosol)), and temperature, while unique factors were Ca2+ in spring and RH in summer. The decreasing SO42- and increasing NO3- mass fractions in PM 2.5 as well as excessive NH3 in the atmosphere in the NCP in recent years are the reasons why aerosol acidity in China is lower than that in Europe and the United States. The nonlinear relationship between PM 2.5 pH and TNH3 indicated that although NH3 in the NCP was abundant, the PM 2.5 pH was still acidic because of the thermodynamic equilibrium between NH4+ and NH3. To reduce nitrate by controlling ammonia, the amount of ammonia must be greatly reduced below excessive quantities. [ABSTRACT FROM AUTHOR]