Ground-level ozone (O3) is a harmful air pollutant formed in the atmosphere by the interaction between sunlight and precursor gases. Exposure to current O3 levels in Europe is a major source of premature mortality from air pollution. However, mitigation actions have been mainly designed and implemented at the national and regional scales, lacking a comprehensive assessment of the geographic sources of O3 pollution and its associated health impacts. Here we quantify both national and imported contributions to O3 and their related mortality burden across 813 contiguous regions in 35 European countries, representing about 530 million people. Imported O3 contributed to 88.3% of all O3-attributable deaths (intercountry range 83-100%). The greatest share of imported O3 had its origins outside the study domain (that is, hemispheric sources), which was responsible for 56.7% of total O3-attributable mortality (range 42.5-87.2%). It was concluded that achieving the air-quality guidelines set out by the World Health Organization and avoiding the health impacts of O3 require not only the implementation of national or coordinated pan-European actions but also global strategies.

Tropospheric ozone impacts health, climate, and ecosystems. Effective ozone mitigation policies are challenged by limited quantitative understanding of national versus transboundary contributions to surface ozone. This study uses a chemical transport model with a source apportionment algorithm to analyze ozone contributions across Europe from 2015 to 2017 during peak ozone season. We quantify country-level ozone production and imported ozone, distinguishing contributions from 35 European countries, neighboring countries, seas, and hemispheric influences. Results show substantial contributions from outside the 35 European countries, with hemispheric contributions playing a significant role. European contributions are crucial during high ozone episodes, especially from Germany, France, Italy, the UK, Poland, and Spain. Spain, northern Italy, and northwest France are identified as areas where national precursor reductions would be more effective in improving national air quality. Furthermore, 25 of the 35 European countries studied are net importers of cumulative ozone mass, with the Netherlands, Belgium, and the UK acting as major exporters. These findings highlight the need for comprehensive air quality policies and cross-border cooperation. The hemispheric transport of air pollutants is a critical external contributor to surface ozone concentration in Europe, and national emissions are key during high concentration episodes, according to an analysis using regional air quality modeling and source apportionment tagging method.

The CALIOPE forecasting system, developed and operated by the Barcelona Supercomputing Center, has been providing daily forecasts of air quality for Europe and Spain since 2008. The system currently integrates an emission processing model (HERMESv3), a meteorological model (WRF-ARW), a chemical transport model (CMAQ), and a mineral dust model (BSC-DREAM8b) that accounts for the dust contribution from North Africa. Since its initial deployment, continuous updates have been implemented to the system, with improvements in emission source estimates and adjustments in the model configuration. Since 2020, and thanks to the co-development with the Catalan Regional Administration and the Barcelona Metropolitan Transport Authority, new approaches and methodologies have been implemented, including a new nested domain at higher spatial resolution (1 × 1 km2) over Catalonia, to further support decision-making. Additionally, beyond the mesoscale domains, the CALIOPE-Urban model has been incorporated into the modelling chain to simulate air quality at the urban street-scale in the city of Barcelona. In parallel to those improvements, the emission estimates have been improved through updates in emission activity data from the industrial and on-road traffic sectors. Lastly, a data-fusion method has been implemented to correct urban air quality fields and reduce biases affecting the forecasting system. In this contribution, we will present the most recent developments applied to the CALIOPE forecasting system and its application as an air quality management tool. We will also discuss future user-driven developments that take both scientific and technical aspects into consideration, including the migration of the mesoscale system to the on-line MONARCH model, a dissemination strategy aiming to promote the wider use of CALIOPE predictions through a new portal designed to improve the user experience, and the further integration of the system into decision-making processes.

Tropospheric ozone (O3) exerts strong adverse impacts on human health, climate, vegetation, biodiversity, agricultural crop yields and thus food security. O3 is formed in the atmosphere through non-linear photochemical reactions between volatile organic compounds (VOCs) and nitrogen oxides (NOx) precursors. Currently, there are no observational methods that differentiate the origin of O3. Despite their inherent uncertainties, chemical transport models (CTMs) allow for the apportionment of the contribution of any source to O3 concentrations. The mass-transfer source apportionment method is an optimal approach to study the contribution of different sources to ozone levels. In this study, we provide a quantitative estimation of the foreign and domestic contributions to ozone among European countries relative to the contribution of hemispheric imported ozone. We use CMAQ-ISAM within the CALIOPE air quality modelling system to simulate the O3 dynamics over Europe at a 18 x 18 km2 horizontal resolution and quantify national contributions for the ozone season from May to October during the years 2015, 2016 and 2017. We tag both O3 and its precursors, NOx and VOCs, from the different European countries, all the way through their lifetime, from emission to deposition. We discuss the results for 35 European countries, including their ozone contribution to other countries, the role of hemispheric background ozone concentrations in each country, and the changes from one year to another.

The application of the multivariate curve resolution method to the analysis of temporal and spatial data variability of hourly measured O3 and NO2 concentrations at nineteen air quality monitoring stations across Catalonia, Spain, during 2015 is shown. Data analyzed included ground-based experimental measurements and predicted concentrations by the CALIOPE air quality modelling system at three horizontal resolutions (Europe at 12 × 12 km2, Iberian Peninsula at 4 × 4 km2 and Catalonia at 1 × 1 km2). Results obtained in the analysis of these different data sets allowed a better understanding of O3 and NO2 concentration changes as a sum of a small number of different contributions related to daily sunlight radiation, seasonal dynamics, traffic emission patterns, and local station environments (urban, suburban and rural). The evaluation of O3 and NO2 concentrations predicted by the CALIOPE system revealed some differences among data sets at different spatial resolutions. NO2 predictions, showed in general a better performance than O3 predictions for the three model resolutions, specially at urban stations. Our results confirmed that the application of the trilinearity constraint during the multivariate curve resolution factor analysis decomposition of the analyzed data sets is a useful tool to facilitate the understanding of the resolved variability sources.

Abstract. The Eurodelta-Trends multi-model experiment, aimed to assess the efficiency of emission mitigation measures in improving air quality in Europe during 1990–2010, was designed to answer a series of questions regarding European pollution trends. i.e. were there significant trends detected by observations? do the models manage to reproduce observed trends? how close is the agreement between the models and how large are the deviations from observations? In this paper, we address these issues with respect to PM pollution. An in-depth trend analysis has been performed for PM10 and PM2.5 for the period of 2000–2010, based on results from six chemical transport models and observational data from the EMEP (Cooperative Programme for Monitoring and Evaluation of the Long-range Transmission of Air Pollutants in Europe) monitoring network. Given harmonization of set up and main input data, the differences in model results should mainly result from differences in the process formulations within the models themselves, and the spread in the models simulated trends could be regarded as an indicator for modelling uncertainty. The model ensemble simulations indicate overall decreasing trends in PM10 and PM2.5, with reduction by between 2 and 6 μg m−3 m−3 (or between 10 and 30 %) from 2000 to 2010. Compared to PM2.5, relative PM10 trends are weaker due to large inter-annual variability of natural coarse PM within the former. The changes in the concentrations of PM individual components are in general consistent with emission reductions. There is a reasonable agreement in PM trends estimated by the individual models, with the inter-model variability below 30–40 % over most of Europe, increasing to 50–60 % in northern and eastern parts of EDT domain. Averaged over measurement sites (26 for PM10 and 13 for PM2.5), the mean ensemble simulated trends are −0.24 and −0.22 μg m−3 year−1 for PM10 and PM2.5, which are somewhat weaker than the observed trends of −0.35 and −0.40 μg m−3 year−1, respectively, partly due to models underestimation of PM concentrations. The correspondence is better in relative PM10 and PM2.5 trends, which are −1.7 and −2.0 % year−1 from the model ensemble and −2.1 and −2.9 % year−1 from the observations, respectively. The observations identify significant trends for PM10 at 56 % of the sites and for PM2.5 at 36 % of the sites, which is somewhat less that the fractions of significant modelled trends. Further, we find somewhat smaller spatial variability of modelled PM trends with respect to the observed ones across Europe and also within individual countries. The strongest decreasing PM trends and the largest number of sites with significant trends is found for the summer season, according to both the model ensemble and observations. The winter PM trends are very weak and mostly insignificant. One important reason for that is the very modest reductions and even increases in the emissions of primary PM from residential heating in winter. It should be kept in mind that all findings regarding modeled versus observed PM trends are limited the regions where the sites are located. The analysis reveals a considerable variability of the role of the individual aerosols in PM10 trends across European countries. The multi-model simulations, supported by available observations, point to decreases in SO4−2 concentrations playing an overall dominant role. Also, we see relatively large contributions of the trends of NH4+ and NO3− to PM10 decreasing trends in Germany, Denmark, Poland and the Po Valley, while the reductions of primary PM emissions appears to be a dominant factor in bringing down PM10 in France, Norway, Portugal, Greece and parts of the UK and Russia. Further discussions are given with respect to emission uncertainties and the effect of inter-annual meteorological variability on the trend analysis.

Background and objective The relationship between IPF development and environmental factors has not been completely elucidated. Analysing geographic regions of idiopathic pulmonary fibrosis (IPF) cases could help identify those areas with higher aggregation and investigate potential triggers. We hypothesize that cross-analysing location of IPF cases and areas of consistently high air pollution concentration could lead to recognition of environmental risk factors for IPF development. Methods This retrospective study analysed epidemiological and clinical data from 503 patients registered in the Observatory IPF.cat from January 2017 to June 2019. Incident and prevalent IPF cases from the Catalan region of Spain were graphed based on their postal address. We generated maps of the most relevant air pollutant PM2.5 from the last 10 years using data from the CALIOPE air quality forecast system and observational data. Results In 2018, the prevalence of IPF differed across provinces; from 8.1 cases per 100 000 habitants in Barcelona to 2.0 cases per 100 000 in Girona. The ratio of IPF was higher in some areas. Mapping PM2.5 levels illustrated that certain areas with more industry, traffic and shipping maintained markedly higher PM2.5 concentrations. Most of these locations correlated with higher aggregation of IPF cases. Compared with other risk factors, PM2.5 exposure was the most frequent. Conclusion In this retrospective study, prevalence of IPF is higher in areas of elevated PM2.5 concentration. Prospective studies with targeted pollution mapping need to be done in specific geographies to compile a broader profile of environmental factors involved in the development of pulmonary fibrosis.

This study aims to quantify the contributions to surface ozone (O3) concentration in the Iberian Peninsula (IP) from the main NOx emission sectors in the region along with the imported O3 during a 10-day episode. The work applies an Integrated Source Apportionment Method within the CALIOPE air quality system at 4-km resolution. This study finds that the imported O3 is overall the larger contribution to its surface concentration. Contributions from local/regional sources are decisive in the O3 peaks downwind of main nitrogen oxides (NOx) hotspots in the IP under stagnant conditions.

The wet deposition of nitrogen and sulfur in Europe for the period 1990–2010 was estimated by six atmospheric chemistry transport models (CHIMERE, CMAQ, EMEP MSC-W, LOTOS-EUROS, MATCH and MINNI) within the framework of the EURODELTA-Trends model intercomparison. The simulated wet deposition and its trends for two 11-year periods (1990–2000 and 2000–2010) were evaluated using data from observations from the EMEP European monitoring network. For annual wet deposition of oxidised nitrogen (WNOx), model bias was within 30 % of the average of the observations for most models. There was a tendency for most models to underestimate annual wet deposition of reduced nitrogen (WNHx), although the model bias was within 40 % of the average of the observations. Model bias for WNHx was inversely correlated with model bias for atmospheric concentrations of NH3+NH4+, suggesting that an underestimation of wet deposition partially contributed to an overestimation of atmospheric concentrations. Model bias was also within about 40 % of the average of the observations for the annual wet deposition of sulfur (WSOx) for most models. Decreasing trends in WNOx were observed at most sites for both 11-year periods, with larger trends, on average, for the second period. The models also estimated predominantly decreasing trends at the monitoring sites and all but one of the models estimated larger trends, on average, for the second period. Decreasing trends were also observed at most sites for WNHx, although larger trends, on average, were observed for the first period. This pattern was not reproduced by the models, which estimated smaller decreasing trends, on average, than those observed or even small increasing trends. The largest observed trends were for WSOx, with decreasing trends at more than 80 % of the sites. On average, the observed trends were larger for the first period. All models were able to reproduce this pattern, although some models underestimated the trends (by up to a factor of 4) and others overestimated them (by up to 40 %), on average. These biases in modelled trends were directly related to the tendency of the models to under- or overestimate annual wet deposition and were smaller for the relative trends (expressed as % yr−1 relative to the deposition at the start of the period). The fact that model biases were fairly constant throughout the time series makes it possible to improve the predictions of wet deposition for future scenarios by adjusting the model estimates using a bias correction calculated from past observations. An analysis of the contributions of various factors to the modelled trends suggests that the predominantly decreasing trends in wet deposition are mostly due to reductions in emissions of the precursors NOx, NH3 and SOx. However, changes in meteorology (e.g. precipitation) and other (non-linear) interactions partially offset the decreasing trends due to emission reductions during the first period but not the second. This suggests that the emission reduction measures had a relatively larger effect on wet deposition during the second period, at least for the sites with observations.

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.

number of relevant references. They also briefly discuss the trends and justify the need for their research. The topic is timely and interesting not only from the scientific point of view but also considering the legal implications and the need to identify potential interventions that may help alleviate O3 pollution in the Mediterranean Basin. Given the limitations of brute force methods for source apportionment studies of secondary pollutants, the authors apply the Integrated Source Apportionment Method (ISAM) implemented within the Community Multiscale Air Quality (CMAQ) with 4x4 km2 resolution for the whole Iberian Peninsula during a 10-day specific episode in summer 2012. The rationale and approach is clear but it would be interesting to explicitly state the main purpose of the study since this is relevant to understand whether the experiment design is appropriate and what are the limitations that can be expected from potential conclusions.

Figure S1: Spatial distribution of the observational sites for SOA (retrieved from PMF analysis).Total number of sites is 48.Sites with averages concentration above 7 µg m -3 over the measuring period were excluded from the analysis.Information on the sites and periods of the measurements are reported in Table S2.

It is well established that in Europe, high O3 concentrations are most pronounced in southern/Mediterranean countries due to the more favourable climatological conditions for its formation. However, the contribution of the different sources of precursors to O3 formation within each country relative to the imported (regional and hemispheric) O3 is poorly quantified. This lack of quantitative knowledge prevents local authorities from effectively designing plans that reduce the exceedances of the O3 target value set by the European air quality directive. O3 source attribution is a challenge because the concentration at each location and time results not only from local biogenic and anthropogenic precursors, but also from the transport of O3 and precursors from neighbouring regions, O3 regional and hemispheric transport and stratospheric O3 injections. The main goal of this study is to provide a first quantitative estimation of the contribution of the main anthropogenic activity sectors to peak O3 events in Spain relative to the contribution of imported (regional and hemispheric) O3. We also assess the potential of our source apportionment method to improve O3 modelling. Our study applies and thoroughly evaluates a countrywide O3 source apportionment method implemented in the CALIOPE air quality forecast system for Spain at high resolution (4 × 4 km2) over a 10-day period characterized by typical summer conditions in the Iberian Peninsula (IP). The method tags both O3 and its gas precursor emissions from source sectors within one simulation, and each tagged species is subject to the typical physico-chemical processes (advection, vertical mixing, deposition, emission and chemistry) as the actual conditions remain unperturbed. We quantify the individual contributions of the largest NOx local sources to high O3 concentrations compared with the contribution of imported O3. We show, for the first time, that imported O3 is the largest input to the ground-level O3 concentration in the IP, accounting for 46 %–68 % of the daily mean O3 concentration during exceedances of the European target value. The hourly imported O3 increases during typical northwestern advections (70 %–90 %, 60–80 µg m−3), and decreases during typical stagnant conditions (30 %–40 %, 30–60 µg m−3) due to the local NO titration. During stagnant conditions, the local anthropogenic precursors control the O3 peaks in areas downwind of the main urban and industrial regions (up to 40 % in hourly peaks). We also show that ground-level O3 concentrations are strongly affected by vertical mixing of O3-rich layers present in the free troposphere, which result from local/regional layering and accumulation, and continental/hemispheric transport. Indeed, vertical mixing largely explains the presence of imported O3 at ground level in the IP. Our results demonstrate the need for detailed quantification of the local and remote contributions to high O3 concentrations for local O3 management, and show O3 source apportionment to be an essential analysis prior to the design of O3 mitigation plans in any non-attainment area. Achieving the European O3 objectives in southern Europe requires not only ad hoc local actions but also decided national and European-wide strategies.

The implementation of European emission abatement strategies has led to a significant reduction in the emissions of ozone precursors during the last decade. Ground-level ozone is also influenced by meteorological factors such as temperature, which exhibit interannual variability and are expected to change in the future. The impacts of climate change on air quality are usually investigated through air-quality models that simulate interactions between emissions, meteorology and chemistry. Within a multi-model assessment, this study aims to better understand how air-quality models represent the relationship between meteorological variables and surface ozone concentrations over Europe. A multiple linear regression (MLR) approach is applied to observed and modelled time series across 10 European regions in springtime and summertime for the period of 2000–2010 for both models and observations. Overall, the air-quality models are in better agreement with observations in summertime than in springtime and particularly in certain regions, such as France, central Europe or eastern Europe, where local meteorological variables show a strong influence on surface ozone concentrations. Larger discrepancies are found for the southern regions, such as the Balkans, the Iberian Peninsula and the Mediterranean basin, especially in springtime. We show that the air-quality models do not properly reproduce the sensitivity of surface ozone to some of the main meteorological drivers, such as maximum temperature, relative humidity and surface solar radiation. Specifically, all air-quality models show more limitations in capturing the strength of the ozone–relative-humidity relationship detected in the observed time series in most of the regions, for both seasons. Here, we speculate that dry-deposition schemes in the air-quality models might play an essential role in capturing this relationship. We further quantify the relationship between ozone and maximum temperature (mo3 − T, climate penalty) in observations and air-quality models. In summertime, most of the air-quality models are able to reproduce the observed climate penalty reasonably well in certain regions such as France, central Europe and northern Italy. However, larger discrepancies are found in springtime, where air-quality models tend to overestimate the magnitude of the observed climate penalty.

Table S1.Detail set up of the CALIOPE system in the present modelling study Meteorological model WRF-ARWv3.5.1 Initial and boundary meteorological conditions GFS-FNL (1.5ºx1.5º,6h) Meteorological spin-up period 12 hours WRF mother domain 12-km resolution over Europe (nx, ny, nz) 480 x 400 x 38 WRF nested domain 4-km resolution over the Iberian Peninsula (nx, ny, nz) 399 x 399 x 38 WRF parametrizations Boundary layer: YSU Microphysics scheme: WSM5 Cumulus scheme: no

The evaluation and intercomparison of air quality models is key to reducing model errors and uncertainty. The projects AQMEII3 and EURODELTA-Trends, in the framework of the Task Force on Hemispheric Transport of Air Pollutants and the Task Force on Measurements and Modelling, respectively (both task forces under the UNECE Convention on the Long Range Transport of Air Pollution, LTRAP), have brought together various regional air quality models to analyze their performance in terms of air concentrations and wet deposition, as well as to address other specific objectives. This paper jointly examines the results from both project communities by intercomparing and evaluating the deposition estimates of reduced and oxidized nitrogen (N) and sulfur (S) in Europe simulated by 14 air quality model systems for the year 2010. An accurate estimate of deposition is key to an accurate simulation of atmospheric concentrations. In addition, deposition fluxes are increasingly being used to estimate ecological impacts. It is therefore important to know by how much model results differ and how well they agree with observed values, at least when comparison with observations is possible, such as in the case of wet deposition. This study reveals a large variability between the wet deposition estimates of the models, with some performing acceptably (according to previously defined criteria) and others underestimating wet deposition rates. For dry deposition, there are also considerable differences between the model estimates. An ensemble of the models with the best performance for N wet deposition was made and used to explore the implications of N deposition in the conservation of protected European habitats. Exceedances of empirical critical loads were calculated for the most common habitats at a resolution of 100 × 100 m2 within the Natura 2000 network, and the habitats with the largest areas showing exceedances are determined. Moreover, simulations with reduced emissions in selected source areas indicated a fairly linear relationship between reductions in emissions and changes in the deposition rates of N and S. An approximate 20 % reduction in N and S deposition in Europe is found when emissions at a global scale are reduced by the same amount. European emissions are by far the main contributor to deposition in Europe, whereas the reduction in deposition due to a decrease in emissions in North America is very small and confined to the western part of the domain. Reductions in European emissions led to substantial decreases in the protected habitat areas with critical load exceedances (halving the exceeded area for certain habitats), whereas no change was found, on average, when reducing North American emissions in terms of average values per habitat.

S1 Analysis of the errors in wet deposition due to errors in the primary particulate matter emissionsErrors were found in the emissions of primary particulate matter for Russia and North African countries and shipping for the period 1991-1999.Unfortunately it was not possible to re-run the simulations since these errors were not detected until late in the data analysis.In order to estimate the impact on the wet deposition estimates, the CHIMERE model was used to simulate wet deposition using the incorrect and corrected emissions for 1998, the year for which the emission error is the largest.Figure S1 shows the relative errors in the model estimates of WNOx, WNHx and WSOx as a result of the errors in emissions.Errors in WNOx and WSOx were less than 0.5% in most of the domain with maximum errors of 0.95% and 1.5%, respectively.Errors in WNHx were also mostly below 0.5% but larger errors were estimated for about a quarter of the domain (mostly in the northeast), with a maximum error of 2.4%.These errors are small compared with the overall uncertainty of the model estimates and the uncertainty of the observations.Errors in the trends calculated from the simulations with erroneous emissions are expected to be smaller than the errors in annual deposition rates.From this analysis we conclude that the error in emissions is unlikely to affect the results and conclusions of the study significantly.Figure S1: Maps of relative difference between the model estimates of WNOx, WNHx and WSOx for the simulations using the original (incorrect) emissions and those using the corrected emissions of primary PM in Russia, North Africa and maritime areas for 1998.Circles show the locations of the sites used to evaluate modelled deposition.Note: Positive values indicate that the emission error resulted in larger values of wet deposition and vice versa. S2 Table and Figures cited in the articleTable S1: Main features of the chemistry-transport models involved in the EURODELTA-Trends deposition modelling exercise (Adapted from Colette et al., 2017a).

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