European Monitoring And Evaluation Programme Research Articles

Impact of methane and other precursor emission reductions on surface ozone in Europe: scenario analysis using the European Monitoring and Evaluation Programme (EMEP) Meteorological Synthesizing Centre – West (MSC-W) model

Abstract. The impacts of future methane (CH4) and other precursor emission changes are investigated for surface ozone (O3) in the United Nations Economic Commission for Europe (UNECE) region excluding North America and Israel (the EMEP region, for European Monitoring and Evaluation Programme) for the year 2050. The analysis includes a current legislation (CLE) and maximum feasible technical reduction (MFR) scenario, as well as a scenario that combines MFRs with an additional dietary shift that also meets the Paris Agreement objectives with respect to greenhouse gas emissions (LOW). For each scenario, background CH4 concentrations are calculated using a probabilistic Earth system model emulator and combined with other precursor emissions in a three-dimensional Eulerian chemistry-transport model. While focus is placed on peak season maximum daily 8 h average (MDA8) O3 concentrations, a range of other indicators for health and vegetation impacts are also discussed. Our analysis shows that roughly one-third of the total peak season MDA8 reduction achieved between the 2050 CLE and MFR scenarios is attributable to CH4 reductions, resulting predominantly from CH4 emission reductions outside of the EMEP region. The impact of other precursor emission reductions is split nearly evenly between the reductions inside and outside of the EMEP region. However, the relative importance of CH4 and other precursor emission reductions is shown to depend on the choice of O3 indicator, though indicators sensitive to peak O3 show generally consistent results. The analysis also highlights the synergistic impacts of CH4 mitigation as reducing solely CH4 achieves, beyond air quality improvement, nearly two-thirds of the total global warming reduction calculated for the LOW scenario compared to the CLE case.

A study of particle dry deposition parameterizations in an atmospheric radioactive preparedness model: Application to the Chernobyl case

Parameterization of dry deposition is key for modelling of atmospheric transport and deposition of radioactive particles. Still, very simple parameterizations are often encountered in radioactive preparedness models such as the SNAP model (SNAP=Severe Nuclear Accident Program) of the Norwegian Meteorological Institute. In SNAP a constant dry deposition velocity (=0.2 cm/s) neglecting aerodynamic and surface resistances, is presently used. Therefore, two new dry depositions schemes (the Emerson scheme and the EMEP (European Monitoring and Evaluation Programme) scheme) have been implemented in SNAP to evaluate the benefits of including aerodynamic and surface resistances codes with respect to model prediction skills. The three dry deposition schemes are evaluated using 137Cs total deposition from soil sample data (n = 540) for a 60 km radial zone out from the Chernobyl Nuclear Power Plant (ChNPP) collected during the months after the accident. The present study capitalizes on high resolution meteorological data (2.5 km horizontal resolution), a detailed land-use data set with 273 sub-classes and the hitherto most comprehensive source term description for the Chernobyl accident. Based on our findings it is recommended to replace the present simple SNAP scheme with the Emerson or EMEP dry deposition scheme.

How well are aerosol–cloud interactions represented in climate models? – Part 1: Understanding the sulfate aerosol production from the 2014–15 Holuhraun eruption

Abstract. For over 6 months, the 2014–2015 effusive eruption at Holuhraun, Iceland, injected considerable amounts of sulfur dioxide (SO2) into the lower troposphere with a daily rate of up to one-third of the global emission rate, causing extensive air pollution across Europe. The large injection of SO2, which oxidises to form sulfate aerosol (SO42-), provides a natural experiment offering an ideal opportunity to scrutinise state-of-the-art general circulation models' (GCMs) representation of aerosol–cloud interactions (ACIs). Here we present Part 1 of a two-part model inter-comparison using the Holuhraun eruption as a framework to analyse ACIs. We use SO2 retrievals from the Infrared Atmospheric Sounding Interferometer (IASI) instrument and ground-based measurements of SO2 and SO42- mass concentrations across Europe, in conjunction with a trajectory analysis using the Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model, to assess the spatial and chemical evolution of the volcanic plume as simulated by five GCMs and a chemical transport model (CTM). IASI retrievals of plume altitude and SO2 column load reveal that the volcanic perturbation is largely contained within the lower troposphere. Compared to the satellite observations, the models capture the spatial evolution and vertical variability of the plume reasonably well, although the models often overestimate the plume altitude. HYSPLIT trajectories are used to attribute to Holuhraun emissions 111 instances of elevated sulfurous surface mass concentrations recorded at European Monitoring and Evaluation Programme (EMEP) stations during September and October 2014. Comparisons with the simulated concentrations show that the modelled ratio of SO2 to SO42- during these pollution episodes is often underestimated and overestimated for the young and mature plume, respectively. Models with finer vertical resolutions near the surface are found to better capture these elevated sulfurous ground-level concentrations. Using an exponential function to describe the decay of observed surface mass concentration ratios of SO2 to SO42- with plume age, the in-plume oxidation rate constant is estimated as 0.032 ± 0.002 h−1 (1.30 ± 0.08 d e-folding time), with a near-vent ratio of 25 ± 5 (µg m−3 of SO2 / µg m−3 of SO42-). The majority of the corresponding derived modelled oxidation rate constants are lower than the observed estimate. This suggests that the representation of the oxidation pathway/s in the simulated plumes is too slow. Overall, despite their coarse spatial resolutions, the six models show reasonable skill in capturing the spatial and chemical evolution of the Holuhraun plume. This capable representation of the underlying aerosol perturbation is essential to enable the investigation of the eruption's impact on ACIs in the second part of this study.

Implementation of the ISORROPIA-lite aerosol thermodynamics model into the EMAC chemistry climate model (based on MESSy v2.55): implications for aerosol composition and acidity

Abstract. This study explores the differences in performance and results by various versions of the ISORROPIA thermodynamic module implemented within the ECHAM/MESSy Atmospheric Chemistry (EMAC) model. Three different versions of the module were used, ISORROPIA II v1, ISORROPIA II v2.3, and ISORROPIA-lite. First, ISORROPIA II v2.3 replaced ISORROPIA II v1 in EMAC to improve pH predictions close to neutral conditions. The newly developed ISORROPIA-lite has been added to EMAC alongside ISORROPIA II v2.3. ISORROPIA-lite is more computationally efficient and assumes that atmospheric aerosols exist always as supersaturated aqueous (metastable) solutions, while ISORROPIA II includes the option to allow for the formation of solid salts at low RH conditions (stable state). The predictions of EMAC by employing all three aerosol thermodynamic models were compared to each other and evaluated against surface measurements from three regional observational networks in the polluted Northern Hemisphere (Interagency Monitoring of Protected Visual Environments (IMPROVE), European Monitoring and Evaluation Programme (EMEP), and Acid Deposition Monitoring Network of East Asia (EANET)). The differences between ISORROPIA II v2.3 and ISORROPIA-lite were minimal in all comparisons with the normalized mean absolute difference for the concentrations of all major aerosol components being less than 11 % even when different phase state assumptions were used. The most notable differences were lower aerosol concentrations predicted by ISORROPIA-lite in regions with relative humidity in the range of 20 % to 60 % compared to the predictions of ISORROPIA II v2.3 in stable mode. The comparison against observations yielded satisfactory agreement especially over the USA and Europe but higher deviations over East Asia, where the overprediction of EMAC for nitrate was as high as 4 µg m−3 (∼20 %). The mean annual aerosol pH predicted by ISORROPIA-lite was on average less than a unit lower than ISORROPIA II v2.3 in stable mode, mainly for coarse-mode aerosols over the Middle East. The use of ISORROPIA-lite accelerated EMAC by nearly 5 % compared to the use of ISORROPIA II v2.3 even if the aerosol thermodynamic calculations consume a relatively small fraction of the EMAC computational time. ISORROPIA-lite can therefore be a reliable and computationally efficient alternative to the previous thermodynamic module in EMAC.

Connection between Weather Types and Air Pollution Levels: A 19-Year Study in Nine EMEP Stations in Spain.

This study focuses on the analysis of the distribution, both spatial and temporal, of the PM10 (particulate matter with a diameter of 10 µm or less) concentrations recorded in nine EMEP (European Monitoring and Evaluation Programme) background stations distributed throughout mainland Spain between 2001 and 2019. A study of hierarchical clusters was used to classify the stations into three main groups with similarities in yearly concentrations: GC (coastal location), GNC (north-central location), and GSE (southeastern location). The highest PM10 concentrations were registered in summer. Annual evolution showed statistically significant decreasing trends in PM10 concentration in all the stations covering a range from -0.21 to -0.50 µg m-3/year for Barcarrota and Víznar, respectively. Through the Lamb classification, the weather types were defined during the study period, and those associated with high levels of pollution were identified. Finally, the values exceeding the limits established by the legislation were analyzed for every station assessed in the study.

Implementation of HONO into the chemistry–climate model CHASER (V4.0): roles in tropospheric chemistry

Abstract. Nitrous acid (HONO) is an important atmospheric gas given its contribution to the cycles of NOx and HOx, but its role in global atmospheric photochemistry is not fully understood. This study implemented three pathways of HONO formation in the chemistry–climate model CHASER (MIROC-ESM) to explore three physical phenomena: gas-phase kinetic reactions (GRs), direct emission (EM), and heterogeneous reactions on cloud and aerosol particles (HRs). We evaluated the simulations by the atmospheric aircraft-based measurements from EMeRGe-Asia-2018 (Effect of Megacities on the Transport and Transformation of Pollutants on the Regional to Global Scales), ATom-1 (atmospheric tomography), observations from the ship R/V Mirai, EANET (Acid Deposition Monitoring Network in eastern Asia)/EMEP (European Monitoring and Evaluation Programme) ground-based stationary observations, and the OMI (Ozone Monitoring Instrument). We showed that the inclusion of the HONO chemistry in the modelling process reduced the model bias against the measurements for PM2.5, NO3-/HNO3, NO2, OH, HO2, O3, and CO, especially in the lower troposphere and the North Pacific (NP) region. We found that the retrieved global abundance of tropospheric HONO was 1.4 TgN. Of the three source pathways, HRs and EM contributed 63 % and 26 % to the net HONO production, respectively. We also observed that reactions on the aerosol surfaces contributed larger amounts of HONO (51 %) than those on the cloud surfaces (12 %). The model exhibited significant negative biases for daytime HONO in the Asian off-the-coast region, compared with the airborne measurements by EMeRGe-Asia-2018, indicating the existence of unknown daytime HONO sources. Strengthening of aerosol uptake of NO2 near the surface and in the middle troposphere, cloud uptake, and direct HONO emission were all potential yet-unknown HONO sources. The most promising daytime source for HONO found in this study was the combination of enhanced aerosol uptake of NO2 and surface-catalysed HNO3 photolysis (maxST+JANO3-B case), which could also remedy the model bias for NO2 and O3 during EMeRGe. We also found that the simulated HONO abundance and its impact on NOx–O3 chemistry were sensitive to the yield of the heterogeneous conversion of NO2 to HONO (vs. HNO3). Inclusion of HONO reduced global tropospheric NOx (NO + NO2) levels by 20.4 %, thereby weakening the tropospheric oxidizing capacity (OH, O3) occurring for NOx-deficit environments (remote regions and upper altitudes), which in turn increased CH4 lifetime (13 %) and tropospheric CO abundance (8 %). The calculated reduction effect on the global ozone level reduced the model overestimates for tropospheric column ozone against OMI spaceborne observations for a large portion of the North Hemisphere. HRs on the surfaces of cloud particles, which have been neglected in previous modelling studies, were the main drivers of these impacts. This effect was particularly salient for the substantial reductions of levels of OH (40 %–67 %) and O3 (30 %–45 %) in the NP region during summer, given the significant reduction of the NOx level (50 %–95 %). In contrast, HRs on aerosol surfaces in China (Beijing) enhanced OH and O3 winter mean levels by 600 %–1700 % and 10 %–33 %, respectively, with regards to their minima in winter. Furthermore, sensitivity simulations revealed that the heterogeneous formation of HONO from NO2 and heterogenous photolysis of HNO3 coincided in the real atmosphere. Nevertheless, the global effects calculated in the combined case (enhancing aerosol uptakes of NO2 and implementing heterogeneous photolysis of HNO3), which most captured the measured daytime HONO level, still reduced the global tropospheric oxidizing capacity. Overall, our findings suggest that a global model that does not consider HONO heterogeneous mechanisms (especially photochemical heterogeneous formations) may erroneously predict the effect of HONO in remote areas and polluted regions.

Comparative Evaluation of the Dynamics of Animal Husbandry Air Pollutant Emissions Using an IoT Platform for Farms

One of the major challenges of animal husbandry, in addition to those related to the economic situation and the current energy crisis, is the major contribution of this sector to atmospheric pollution. Awareness of pollution sources and their permanent monitoring in order to ensure efficient management of the farm, with the aim of reducing emissions, is a mandatory issue, both at the macro level of the economic sector and at the micro level, specifically at the level of each individual farm. In this context, the acquisition of consistent environmental data from the level of each farm will constitute a beneficial action both for the decision-making system of the farm and for the elaboration or adjustment of strategies at the national level. The current paper proposes a case study of air pollutants in a cattle farm for different seasons (winter and summer) and the correlation between their variation and microclimate parameters. A further comparison is made between values estimated using the EMEP (European Monitoring and Evaluation Programme, 2019) methodology for air pollutant emission and values measured by sensors in a hybrid decision support platform for farms. Results show that interactions between microclimate and pollutant emissions exist and they can provide a model for the farm’s activities that the farmer can manage according to the results of the measurements.

Modelling the Impact of the Introduction of the EURO 6d-TEMP/6d Regulation for Light-Duty Vehicles on EU Air Quality

In this manuscript, we evaluated different emission scenarios for light-duty road transport to evaluate their impact on air quality in the EU, with a focus on a number of cities by means of the EMEP (European Monitoring and Evaluation Programme) modelling system. In addition to the reference case scenario, where exhaust emission factors from COPERT (Computer Programme to calculate Emissions from Road Transport) corresponding to the existing fleet were used, we also tested future potential scenarios considering: (a) all passenger cars and light commercial vehicles meet the EURO 6 emissions standard and EDGAR (Emission Database for Global Atmospheric research) EURO 6 emission factors; (b) all passenger cars and light commercial vehicles meet the EURO 6 emissions standard and real-world emission factors derived from actual Euro 6d-TEMP/6d vehicles. Results show how the replacement of old vehicles by newer ones with better emission control technologies can help improve air quality in the EU in terms of reductions in NO2 and PM2.5 concentrations. However, reduced NOx emissions in cities (as foreseen in the two scenarios analysed) will cause tropospheric O3 to increase.

Atmospheric composition in the European Arctic and 30 years of the Zeppelin Observatory, Ny-Ålesund

Abstract. The Zeppelin Observatory (78.90∘ N, 11.88∘ E) is located on Zeppelin Mountain at 472 m a.s.l. on Spitsbergen, the largest island of the Svalbard archipelago. Established in 1989, the observatory is part of Ny-Ålesund Research Station and an important atmospheric measurement site, one of only a few in the high Arctic, and a part of several European and global monitoring programmes and research infrastructures, notably the European Monitoring and Evaluation Programme (EMEP); the Arctic Monitoring and Assessment Programme (AMAP); the Global Atmosphere Watch (GAW); the Aerosol, Clouds and Trace Gases Research Infrastructure (ACTRIS); the Advanced Global Atmospheric Gases Experiment (AGAGE) network; and the Integrated Carbon Observation System (ICOS). The observatory is jointly operated by the Norwegian Polar Institute (NPI), Stockholm University, and the Norwegian Institute for Air Research (NILU). Here we detail the establishment of the Zeppelin Observatory including historical measurements of atmospheric composition in the European Arctic leading to its construction. We present a history of the measurements at the observatory and review the current state of the European Arctic atmosphere, including results from trends in greenhouse gases, chlorofluorocarbons (CFCs) and hydrochlorofluorocarbons (HCFCs), other traces gases, persistent organic pollutants (POPs) and heavy metals, aerosols and Arctic haze, and atmospheric transport phenomena, and provide an outline of future research directions.

Уточнение данных о землепользовании для расчетов эмиссий в химической транспортной модели CHIMERE на примере нижегородского региона

Refinement of land use data for emission calculations in the CHIMERE chemistry-transport model: A case study for the Nizhny Novgorod region / Borisov D.V., Shalygina I.U. // Hydrometeorological Research and Forecasting, 2021, no. 3 (381), pp. 150-161. The quality of calculating the concentration of pollutants in the chemistry-transport model largely depends on the reliability of used emission data. The possibility of updating the EMEP (European Monitoring and Evaluation Program) emission data using OpenStreetMap geodata for the CHIMERE chemistry-transport model calculations is discussed on the example of the Nizhny Novgorod region. The GlobCover land-use data refinement procedure based on OpenStreetMap information provides a 3.3% increase in the urban area and a more accurate configuration of the emission field as compared to the real distribution of sources of atmospheric emissions. Experimental CHIMERE chemistry-transport model calculations of pollutant concentrations based on the initial and updated emission fields demonstrated the efficiency of the proposed approach. Keywords: emissions, EMEP, land use, OpenStreetMap, CHIMERE chemistry-transport model, air quality

Atmospheric ammonia and nitrogen deposition on Irish Natura 2000 sites: Implications for Irish agriculture

With growing global demand for food, the agriculture sector worldwide is under pressure to intensify and expand, risking acceleration of existing negative biodiversity impacts. Agriculture is the dominant source of ammonia (NH3) emissions, which can impact biodiversity directly through dry deposition as NH3 and by wet deposition following conversion to ammonium (NH4) in the atmosphere. Nitrogen deposition is one of the leading causes of global decline in biodiversity alongside changing land use and climate. Natura 2000 sites which are intended to protect important habitats and species across Europe, require strict levels of protection to ensure designated features achieve favourable conservation status. Many of these sites are nitrogen-limited, and/or contain sensitive species such as lichens or mosses. This project carried out ambient NH3 monitoring on selected Irish Natura 2000 sites, in order to establish potential impacts from agricultural NH3. Monitoring on twelve Natura 2000 sites observed concentrations ranging from 0.47 to 4.59 μg NH3 m−3, from which dry deposition was calculated to be 1.22–11.92 kg N ha−1 yr−1. European Monitoring and Evaluation Programme (EMEP) was used to quantify wet deposited NH4 and nitrogen oxides (NOx), in addition to dry deposited NOx on monitored sites. Estimated total nitrogen deposition ranged between 5.93 and 17.78 kg N ha−1 yr−1. On average across all monitored sites, deposition was comprised of 50.4%, 31.7%, 7.5%, and 10.3% dry NH3, wet NH4, dry NOx and wet NOx respectively. Implications for Irish agriculture are discussed in the light of both this monitoring and the European Commission Dutch Nitrogen Case (C 293/17 & C 294/17), highlighting a number of recommendations to aid compliance with the EU Habitats Directive (92/43/EEC).

Long-term time trend of lead exposure in young German adults - Evaluation of more than 35Years of data of the German Environmental Specimen Bank.

Lead is a ubiquitous pollutant with well-known effects on human health. As there is no lower toxicological threshold for lead in blood and since data gaps on lead exposure still exist in many European countries, HBM data on lead is of high importance. To address this, the European Human Biomonitoring Initiative HBM4EU classified lead as a priority substance. The German Environmental Specimen Bank (German ESB) has monitored lead exposure since more than 35 years. Using data from the early 1980s to 2019 we reveal and discuss long-term trends in blood lead levels (BLLs) and current internal exposure of young adults in Germany. BLLs in young adults decreased substantially in the investigated period. As results from the ESB sampling site Muenster demonstrate, the geometric mean of BLLs of young adults decreased from 1981 (78,7μg/L) to 2019 (10.4μg/L) by about 87%. Trends in human exposure closely correlate with air lead levels (ALLs) provided by the European Monitoring and Evaluation Programme (EMEP). Hence, the decrease of BLLs largely reflects the drop in air lead pollution. Known associations of sex, smoking, alcohol consumption, and housing situation with BLLs are confirmed with data of the German ESB. Although internal lead exposure in Germany decreased substantially, the situation might be different in other European countries. Since 2010, BLLs of young adults in Germany levelled out at approximately 10μg/L. The toxicity of lead even at low levels is known to cause adverse health effects especially in children following exposure of the child or the mother during pregnancy. To identify current exposure sources and to minimize future lead exposure, continuous monitoring of lead intake and exposure levels is needed.

Impacts of Droughts and Acidic Deposition on Long-Term Surface Water Dissolved Organic Carbon Concentrations in Upland Catchments in Wales

Concerns have been raised about rising trends in surface water dissolved organic carbon (DOC) concentrations in UK upland catchments over the past decades. Several mechanisms have been proposed to explain these trends, including changes in climate and declines in sulphate deposition across Europe. Drier summers and wetter winters are projected in the UK, and there is an increasing interest in whether the rising trends of DOC would be continued or stabilised. In this paper, the INCA (INtegrated CAtchment) water quality model was applied to the upland catchment of the River Severn at Plynlimon in Wales and used to simulate the effects of both climate and sulphate deposition on surface water DOC concentrations. We introduced new parameter sets of INCA to explain enzymatic latch effect in peatlands during droughts. The model was able to simulate recent past (1995-2013) rising trends in DOC in Plynlimon. Climatic projections were employed to estimate the future trends on DOC in the uplands and to consider potential impacts on catchment management. The model was run with climatic scenarios generated using the weather@home2 climate modelling platform and with sulphate deposition scenarios from the European Monitoring and Evaluation Programme (EMEP) for 1975-2100. The modelling results show that the rising DOC trends are likely to continue in the near future (2020-2049) and the level of DOC concentrations is projected to stabilise in the far future (2070-2099). However, in the far future, the seasonal patterns of DOC concentrations will change, with a post-drought DOC surge in autumn months.

Characterization of long-range transported bioaerosols in the Central Mediterranean

Airborne bacteria were characterized over a 2-y period via high-throughput massive sequencing of 16S rRNA gene in aerosol samples collected at a background mountain European Monitoring and Evaluation Programme (EMEP) Network site (Monte Martano, Italy) located in the Central Mediterranean area. The air mass origin of nineteen samples was identified by air mass modelling and a detailed chemical analysis was performed. Four main origins (Saharan, North-western, North-eastern, and Regional) were identified, and distinct microbial communities were associated with these air masses. Samples featured a great bacterial diversity with Protobacteria being the most abundant phylum, and Sphingomonas followed by Acidovorax, Acinetobacter and Stenotrophomonas the most abundant genera of the dataset. Bacterial genera including potential human and animal pathogens were more abundant in European and in Regional samples compared to Saharan samples; this stressed the relevance of anthropic impact on bacterial populations transported by air masses that cross densely populated areas. The principal aerosol chemical characteristics and the airborne bacterial communities were correlated by cluster analysis, similarity tests and non-metric multidimensional scaling analysis, explaining most of the variability observed. However, the strong correlation between bacterial community structure and air mass origin hampered the possibility to disentangle the effects of variations in bacterial populations and in dust provenance on variations in chemical variables.

Long-Term Temporal Changes of Precipitation Quality in Slovak Mountain Forests

The paper is focused on the evaluation of long-term changes in the chemical composition of precipitation in the mountain forests of Slovakia. Two stations with long-term measurements of precipitation quality were selected, namely the station of the EMEP (European Monitoring and Evaluation Programme) network Chopok (2008 m a.s.l.) and the station of the ICP Forests (International Co-operative Programme on Assessment and Monitoring of Air Pollution Effects on Forests) network Poľana-Hukavský grúň (850 m a.s.l.). All basic chemical components were analyzed, namely sulfur (S-SO4), nitrogen (N-NH4, N-NO3), and base cations (Ca, Mg, and K) contained in precipitation. The time changes of the individual components were statistically evaluated by the Mann–Kendall test and Kruskal–Wallis test. The results showed significant declining trends for almost all components, which can significantly affect element cycles in mountain forest ecosystems. The evaluated forty one-year period (1987 to 2018) is characterized by significant changes in the precipitation regime in Slovakia and the obtained results indicate possible directions in which the quantity and quality of precipitation in the mountainous areas of Slovakia will develop with ongoing climate change.

Chemical Composition of Atmospheric Aerosol in the Arctic Region and Adjoining Seas along the Routes of Marine Expeditions in 2018–2019

We consider the chemical composition (ions, elements, and polycyclic aromatic hydrocarbons) of atmospheric aerosol in different regions of the North Atlantic, European and Russian parts of the Arctic Ocean, and northern latitude and Far East seas. The studies were carried out onboard marine ships along their cruising routes (RV Akademik Tryoshnikov, RV Akademik Mstislav Keldysh, and RV Professor Multanovsky). The air samples were collected using the method accepted in the international networks operating under the Acid Deposition Monitoring Network in East Asia (EANET) and European Monitoring and Evaluation Programme (EMEP). The average sum of ion concentrations and the concentrations of individual ions in the aerosol over the seas in the North Atlantic and in the European part of the Arctic Ocean is consistent with measurements in the Laptev and Kara Seas in 2018 and 2019. The high concnetrations of PAHs in aerosol in seas and the Arctic Ocean in the central part of the Russian Arctic coincide with high concentrations of ions and trace elements in the aerosol composition. A difference is noted in the distribution of concentrations of trace elements in aerosol composition between seas of the North Atlantic and central region of the Russian Arctic, which possibly points to different sources of these components.

Long term trends of wet deposition and atmospheric concentrations of nitrogen and sulfur compounds at EMEP site in Armenia

This paper presents the trends of gaseous nitric acid, nitrogen dioxide, sulfur dioxide, ammonia and nitrate, ammonium, sulfate ions in atmospheric air, and nitrate, ammonium and sulfate ions in wet deposition over 2008–2018 in Armenia. Atmospheric nitrogen and sulfur concentrations were monitored by data obtained from filter pack samplers and glass sinter filters at background monitoring station of Armenia (Amberd), which is designated as EMEP (European Monitoring and Evaluation Programme) station. Laboratory analyses were performed by ion chromatography system and UV spectrophotometer. MAKESENS programme was used for detecting and estimating trends in the time series of annual average values of atmospheric concentrations. Long term trends of atmospheric concentrations of nitrogen and sulfur compounds at the Amberd air quality monitoring station were calculated and discussed for the investigated decade. The trends significance levels for all parameters are calculated. It is identified that there are no significant trends for all explored paramenters, except reduced sulfur in aerosols. Possible emission and deposition changes of nitrogen and sulfur compounds in Armenia were explored in order to identify possible transboundary air pollution and its main sources. Deposition data was estimated by EMEP MSC-W model calculations. Investigation of transboundary fluxes of nitrogen and sulfur compounds displays main receptor areas and contributors. Analysis of seasonality in atmospheric pollutants shows strong seasonal behaviour of the measured parameters in wet deposition - higher concentrations during summertime compared with the wintertime. Atmospheric concentrations of nitrate and ammonium ions are lower during summertime compared with the wintertime, while ammonia has low concentrations during wintertime. Atmospheric nitric acid, sulfate ion, sulfur dioxide and nitrogen dioxide revel no significant seasonality.

The Effect of Emission Inventory on Modelling of Seasonal Exposure Metrics of Particulate Matter and Ozone with the WRF-Chem Model for Poland

In Poland, high concentrations of particulate matter (with a diameter smaller than 2.5 or 10 μm) exceeding the WHO threshold values are often measured in winter, while ozone (O3) concentrations are high in spring. In winter high PM2.5 and PM10 concentrations are linked to high residential combustion and road transport. The main objective of this study was to assess performance of the Weather Research and Forecasting model with Chemistry (WRF-Chem) model in reproducing observations for a period of 2017-2018 covering various meteorological conditions. We compare modelled and observed exposure metrics for PM2.5, PM10 and O3 for two sets of the WRF-Chem model runs: with coarse and fine resolution emission inventory (European Monitoring and Evaluation Programme (EMEP) and Chief Inspectorate of Environmental Protection (CIEP), respectively). CIEP run reduces the negative bias of PM2.5 and PM10 and improves the model performance for number of days with exceedance of WHO (World Health Organization) threshold for PM2.5 and PM10 24-h mean concentration. High resolution emission inventory for primary aerosols helps to better distinguish polluted urban areas from non-urban ones. There are no large differences for the model performance for O3 and secondary inorganic aerosols, and high-resolution emission inventory does not improve the results in terms of 8-h rolling mean concentrations of ozone.

Reconstructing Elemental Carbon Long-Term Trend in the Po Valley (Italy) from Fog Water Samples

Elemental carbon (EC), a ubiquitous component of fine atmospheric aerosol derived from incomplete combustion, is an important player for both climate change and air quality deterioration. Several policy measures have been implemented over the last decades to reduce EC emissions from anthropogenic sources, but still, long-term EC measurements to verify the efficacy of such measurements are limited. In this study, we analyze the concentration of EC suspended in fog water samples, collected over the period 1997–2016 in a rural background site of the southern Po Valley. The comparison between EC in fog water and EC atmospheric aerosol concentration measured since 2012 allowed us to reconstruct EC atmospheric concentration from fog water chemical composition dating back to 1997. The results agree with the EC atmospheric observations performed at the European Monitoring and Evaluation Program (EMEP) station of Ispra in the northern part of the Po Valley since 2002, and confirm that the Po Valley is a pollution hotspot, not only in urban areas, but also in rural locations. The reconstructed trend over the period 1997–2016 indicates that EC concentration during the winter season has decreased on average by 4% per year, in agreement with the emission reduction rate, confirming the effectiveness of air quality measures implemented during the past 20 years.

Large-scale particulate air pollution and chemical fingerprint of volcanic sulfate aerosols from the 2014–2015 Holuhraun flood lava eruption of Bárðarbunga volcano (Iceland)

Abstract. Volcanic sulfate aerosols play a key role in air quality and climate. However, the rate of oxidation of sulfur dioxide (SO2) precursor gas to sulfate aerosols (SO42-) in volcanic plumes is poorly known, especially in the troposphere. Here we determine the chemical speciation as well as the intensity and temporal persistence of the impact on air quality of sulfate aerosols from the 2014–2015 Holuhraun flood lava eruption of Icelandic volcano Bárðarbunga. To do so, we jointly analyse a set of SO2 observations from satellite (OMPS and IASI) and ground-level measurements from air quality monitoring stations together with high temporal resolution mass spectrometry measurements of an Aerosol Chemical Speciation Monitor (ACSM) performed far from the volcanic source. We explore month/year long ACSM data in France from stations in contrasting environments, close and far from industrial sulfur-rich activities. We demonstrate that volcanic sulfate aerosols exhibit a distinct chemical signature in urban/rural conditions, with NO3:SO4 mass concentration ratios lower than for non-volcanic background aerosols. These results are supported by thermodynamic simulations of aerosol composition, using the ISORROPIA II model, which show that ammonium sulfate aerosols are preferentially formed at a high concentration of sulfate, leading to a decrease in the production of particulate ammonium nitrate. Such a chemical signature is however more difficult to identify at heavily polluted industrial sites due to a high level of background noise in sulfur. Nevertheless, aged volcanic sulfates can be distinguished from freshly emitted industrial sulfates according to their contrasting degree of anion neutralization. Combining AERONET (AErosol RObotic NETwork) sunphotometric data with ACSM observations, we also show a long persistence over weeks of pollution in volcanic sulfate aerosols, while SO2 pollution disappears in a few days at most. Finally, gathering 6-month long datasets from 27 sulfur monitoring stations of the EMEP (European Monitoring and Evaluation Programme) network allows us to demonstrate a much broader large-scale European pollution, in both SO2 and SO4, associated with the Holuhraun eruption, from Scandinavia to France. While widespread SO2 anomalies, with ground-level mass concentrations far exceeding background values, almost entirely result from the volcanic source, the origin of sulfate aerosols is more complex. Using a multi-site concentration-weighted trajectory analysis, emissions from the Holuhraun eruption are shown to be one of the main sources of SO4 at all EMEP sites across Europe and can be distinguished from anthropogenic emissions from eastern Europe but also from Great Britain. A wide variability in SO2:SO4 mass concentration ratios, ranging from 0.8 to 8.0, is shown at several stations geographically dispersed at thousands of kilometres from the eruption site. Despite this apparent spatial complexity, we demonstrate that these mass oxidation ratios can be explained by a simple linear dependency on the age of the plume, with a SO2-to-SO4 oxidation rate of 0.23 h−1. Most current studies generally focus on SO2, an unambiguous and more readily measured marker of the volcanic plume. However, the long persistence of the chemical fingerprint of volcanic sulfate aerosols at continental scale, as shown for the Holuhraun eruption here, casts light on the impact of tropospheric eruptions and passive degassing activities on air quality, health, atmospheric chemistry and climate.