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Numerical methods and simulation codes are essential for the advancement of our understanding of complex atmospheric processes. As technology and computer hardware continue to evolve, the development of sophisticated code is vital for accurate and efficient simulations. In this paper, we present the recent advancements made in the FLEXible PARTicle dispersion model (FLEXPART), a Lagrangian particle dispersion model, which has been used in a wide range of atmospheric transport studies over the past 3 decades, extending from tracing radionuclides from the Fukushima nuclear disaster, to inverse modelling of greenhouse gases, and to the study of atmospheric moisture cycles. This version of FLEXPART includes notable improvements in accuracy and computational efficiency. (1) By leveraging the native vertical coordinates of European Centre for Medium Range Weather Forecasts (ECMWF) Integrated Forecasting System (IFS) instead of interpolating to terrain-following coordinates, we achieved an improvement in trajectory accuracy, leading to a ∼8 %–10 % reduction in conservation errors for quasi-conservative quantities like potential vorticity. (2) The shape of aerosol particles is now accounted for in the gravitational settling and dry-deposition calculation, increasing the simulation accuracy for non-spherical aerosol particles such as microplastic fibres. (3) Wet deposition has been improved by the introduction of a new below-cloud scheme, by a new cloud identification scheme, and by improving the interpolation of precipitation. (4) Functionality from a separate version of FLEXPART, the FLEXPART CTM (chemical transport model), is implemented, which includes linear chemical reactions. Additionally, the incorporation of Open Multi-Processing parallelisation makes the model better suited for handling large input data. Furthermore, we introduced novel methods for the input and output of particle properties and distributions. Users now have the option to run FLEXPART with more flexible particle input data, providing greater adaptability for specific research scenarios (e.g. effective backward simulations corresponding to satellite retrievals). Finally, a new user manual (https://flexpart.img.univie.ac.at/docs/, last access: 11 September 2024) and restructuring of the source code into modules will serve as a basis for further development.

We analyzed long-term measurements of organic carbon, elemental carbon, and source-specific organic tracers from 2017 to 2020 to constrain carbonaceous aerosol sources in the rapidly changing Arctic. Additionally, we used absorption photometer (Aethalometer) measurements to constrain equivalent black carbon (eBC) from biomass burning and fossil fuel combustion, using positive matrix factorization (PMF). Our analysis shows that organic tracers are essential for understanding Arctic carbonaceous aerosol sources. Throughout 2017 to 2020, levoglucosan exhibited bimodal seasonality, reflecting emissions from residential wood combustion (RWC) in the heating season (November to May) and from wildfires (WFs) in the non-heating season (June to October), demonstrating a pronounced interannual variability in the influence of WF. Biogenic secondary organic aerosol (BSOA) species (2-methyltetrols) from isoprene oxidation was only present in the non-heating season, peaking in July to August. Warm air masses from Siberia led to a substantial increase in 2-methyltetrols in 2019 and 2020 compared to 2017 to 2018. This highlights the need to investigate the contribution of local sources vs. long-range atmospheric transport (LRT), considering the temperature sensitivity of biogenic volatile organic compound emissions from Arctic vegetation. Tracers of primary biological aerosol particles (PBAPs), including various sugars and sugar alcohols, showed elevated levels in the non-heating season, although with different seasonal trends, whereas cellulose had no apparent seasonality. Most PBAP tracers and 2-methyltetrols peaked during influence of WF emissions, highlighting the importance of measuring a range of source-specific tracers to understand sources and dynamics of carbonaceous aerosol. The seasonality of carbonaceous aerosol was strongly influenced by LRT episodes, as background levels are extremely low. In the non-heating season, the organic aerosol peak was as influenced by LRT, as was elemental carbon during the Arctic haze period. Source apportionment of carbonaceous aerosol by Latin hypercube sampling showed mixed contributions from RWC (46 %), fossil fuel (FF) sources (27 %), and BSOA (25 %) in the heating season. In contrast, the non-heating season was dominated by BSOA (56 %), with lower contributions from WF (26 %) and FF sources (15 %). Source apportionment of eBC by PMF showed that FF combustion dominated eBC (70±2.7 %), whereas RWC (22±2.7 %) was more abundant than WF (8.0±2.9 %). Modeled BC concentrations from FLEXPART (FLEXible PARTicle dispersion model) attributed an almost equal share to FF sources (51±3.1 %) and to biomass burning. Both FLEXPART and the PMF analysis concluded that RWC is a more important source of (e)BC than WF. However, with a modeled RWC contribution of 30±4.1 % and WF of 19±2.8 %, FLEXPART suggests relatively higher contributions to eBC from these sources. Notably, the BB fraction of EC was twice as high as that of eBC, reflecting methodological differences between source apportionment by LHS and PMF. However, important conclusions drawn are unaffected, as both methods indicate the presence of RWC- and WF-sourced BC at Zeppelin, with a higher relative BB contribution during the non-heating season. In summary, organic aerosol (281±106 ng m−3) constitutes a significant fraction of Arctic PM10, although surpassed by sea salt aerosol (682±46.9 ng m−3), mineral dust (613±368 ng m−3), and typically non-sea-salt sulfate SO42- (314±62.6 ng m−3), originating mainly from anthropogenic sources in winter and from natural sources in summer.

Ammonia (NH3), a significant precursor of particulate matter, affects not only biodiversity, ecosystems, and soil acidification but also climate and human health. In addition, its concentrations are constantly rising due to increasing feeding needs and the large use of fertilization and animal farming. Despite the significance of ammonia, its emissions are associated with large uncertainties, while its atmospheric abundance is difficult to measure. Nowadays, satellite products can effectively measure ammonia with low uncertainty and a global coverage. Here, we use satellite observations of column ammonia in combination with an inversion algorithm to derive ammonia emissions with a high resolution over Europe for the period 2013–2020. Ammonia emissions peak in northern Europe due to agricultural application and livestock management, in western Europe (industrial activity), and over Spain (pig farming). Emissions have decreased by −26 % since 2013 (from 5431 Gg in 2013 to 3994 Gg in 2020), showing that the abatement strategies adopted by the European Union have been very efficient. The slight increase (+4.4 %) in 2015 is also reproduced here and is attributed to some European countries exceeding annual emission targets. Ammonia emissions are low in winter (286 Gg) and peak in summer (563 Gg) and are dominated by the temperature-dependent volatilization of ammonia from the soil. The largest emission decreases were observed in central and eastern Europe (−38 %) and in western Europe (−37 %), while smaller decreases were recorded in northern (−17 %) and southern Europe (−7.6 %). When complemented with ground observations, modelled concentrations using the posterior emissions showed improved statistics, also following the observed seasonal trends. The posterior emissions presented here also agree well with respective estimates reported in the literature and inferred from bottom-up and top-down methodologies. These results indicate that satellite measurements combined with inverse algorithms constitute a robust tool for emission estimates and can infer the evolution of ammonia emissions over large timescales.

Brominated flame retardants (BFRs) that are gradually being phased out are being replaced by emerging BFRs. Here, we report the concentration of the α- and β-isomers of 1,2-dibromo-4-(1,2-dibromoethyl)cyclohexane (TBECH; also known as DBE-DBCH) in over 300 air, water, and precipitation samples collected between 2019 and 2022 using active air and deposition sampling as well as networks of passive air and water samplers. The sampling region includes Canada's most populated cities and areas along the St. Lawrence River and Estuary, Quebec, as well as around the Salish Sea, British Columbia. TBECH was detected in over 60 % of air samples at levels comparable to those of 2,2′,4,4′-tetrabromodiphenyl ether (BDE-47). Concentrations of TBECH and BDE-47 were typically higher in urban areas, with stronger correlations with population density during warmer deployments. Uniform α- / β-TBECH ratios across space, time, and environmental media indicate the highly similar atmospheric fate of the two isomers. Although TBECH air concentrations were strongly related to temperature in urban Toronto and a remote site on the east coast, the lack of such dependence at a remote site on the west coast can be explained by the small seasonal temperature range and summertime air mass transport from the Pacific Ocean. Despite there being no evidence that TBECH has been produced, or imported for use, in Canada, it is now one of the most abundant gaseous BFRs in the Canadian atmosphere. The recorded spatial and temporal variability of TBECH suggest that its emissions are not constrained to specific locations but are generally tied to the presence of humans. The most likely explanation for its environmental occurrence in Canada is the release from imported consumer products containing TBECH. Chiral analysis suggests that despite its urban origin, at least some fraction of TBECH has experienced enantioselective processing, i.e., has volatilized from reservoirs where it has undergone microbial transformations. Microbial processes in urban soils and in marine waters may have divergent enantioselectivity.

Individual high-Alpine ice cores have been proven to contain a well-preserved history of past anthropogenic air pollution in western Europe. The question of how representative one ice core is with respect to the reconstruction of atmospheric composition in the source region has not been addressed so far. Here, we present the first study systematically comparing longer-term ice-core records (1750–2015 CE) of various anthropogenic compounds, such as major inorganic aerosol constituents (NH4+, NO3-, SO42-), black carbon (BC), and trace species (Cd, F−, Pb). Depending on the data availability for the different air pollutants, up to five ice cores from four high-Alpine sites located in the European Alps analysed by different laboratories were considered. Whereas absolute concentration levels can partly differ depending on the prevailing seasonal distribution of accumulated precipitation, all seven investigated anthropogenic compounds are in excellent agreement between the various sites for their respective, species-dependent longer-term concentration trends. This is related to common source regions of air pollution impacting the four sites less than 100 km away including western European countries surrounding the Alps. For individual compounds, the Alpine ice-core composites developed in this study allowed us to precisely time the onset of pollution caused by industrialization in western Europe. Extensive emissions from coal combustion and agriculture lead to an exceeding of pre-industrial (1750–1850) concentration levels already at the end of the 19th century for BC, Pb, exSO42- (non-dust, non-sea salt SO42-), and NH4+, respectively. However, Cd, F−, and NO3- concentrations started surpassing pre-industrial values only in the 20th century, predominantly due to pollution from zinc and aluminium smelters and traffic. The observed maxima of BC, Cd, F−, Pb, and exSO42- concentrations in the 20th century and a significant decline afterwards clearly reveal the efficiency of air pollution control measures such as the desulfurization of coal, the introduction of filters and scrubbers in power plants and metal smelters, and the ban of leaded gasoline improving the air quality in western Europe. In contrast, NO3- and NH4+ concentration records show levels in the beginning of the 21th century which are unprecedented in the context of the past 250 years, indicating that the introduced abatement measures to reduce these pollutants were insufficient to have a major effect at high altitudes in western Europe. Only four ice-core composite records (BC, F−, Pb, exSO42-) of the seven investigated pollutants correspond well with modelled trends, suggesting inaccuracies of the emission estimates or an incomplete representation of chemical reaction mechanisms in the models for the other pollutants. Our results demonstrate that individual ice-core records from different sites in the European Alps generally provide a spatially representative signal of anthropogenic air pollution trends in western European countries.

While carbon dioxide is the main cause for global warming, modeling short-lived climate forcers (SLCFs) such as methane, ozone, and particles in the Arctic allows us to simulate near-term climate and health impacts for a sensitive, pristine region that is warming at 3 times the global rate. Atmospheric modeling is critical for understanding the long-range transport of pollutants to the Arctic, as well as the abundance and distribution of SLCFs throughout the Arctic atmosphere. Modeling is also used as a tool to determine SLCF impacts on climate and health in the present and in future emissions scenarios. In this study, we evaluate 18 state-of-the-art atmospheric and Earth system models by assessing their representation of Arctic and Northern Hemisphere atmospheric SLCF distributions, considering a wide range of different chemical species (methane, tropospheric ozone and its precursors, black carbon, sulfate, organic aerosol, and particulate matter) and multiple observational datasets. Model simulations over 4 years (2008–2009 and 2014–2015) conducted for the 2022 Arctic Monitoring and Assessment Programme (AMAP) SLCF assessment report are thoroughly evaluated against satellite, ground, ship, and aircraft-based observations. The annual means, seasonal cycles, and 3-D distributions of SLCFs were evaluated using several metrics, such as absolute and percent model biases and correlation coefficients. The results show a large range in model performance, with no one particular model or model type performing well for all regions and all SLCF species. The multi-model mean (mmm) was able to represent the general features of SLCFs in the Arctic and had the best overall performance. For the SLCFs with the greatest radiative impact (CH4, O3, BC, and SO42-), the mmm was within ±25 % of the measurements across the Northern Hemisphere. Therefore, we recommend a multi-model ensemble be used for simulating climate and health impacts of SLCFs. Of the SLCFs in our study, model biases were smallest for CH4 and greatest for OA. For most SLCFs, model biases skewed from positive to negative with increasing latitude. Our analysis suggests that vertical mixing, long-range transport, deposition, and wildfires remain highly uncertain processes. These processes need better representation within atmospheric models to improve their simulation of SLCFs in the Arctic environment. As model development proceeds in these areas, we highly recommend that the vertical and 3-D distribution of SLCFs be evaluated, as that information is critical to improving the uncertain processes in models.

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.

In early October 2020, northern Europe experienced an episode with poor air quality due to high concentrations of particulate matter (PM). At several sites in Norway, recorded weekly values exceeded historical maximum PM10 concentrations from the past 4 to 10 years. Daily mean PM10 values at Norwegian sites were up to 97 µg m−3 and had a median value of 59 µg m−3. We analysed this severe pollution episode caused by long-range atmospheric transport based on surface and remote sensing observations and transport model simulations to understand its causes. Samples from three sites in mainland Norway and the Arctic remote station Zeppelin (Svalbard) showed strong contributions from mineral dust to PM10 (23 %–36 % as a minimum and 31 %–45 % as a maximum) and biomass burning (8 %–16 % to 19 %–21 %). Atmospheric transport simulations indicate that Central Asia was the main source region for mineral dust observed in this episode. The biomass burning fraction can be attributed to forest fires in Ukraine and southern Russia, but we cannot exclude other sources contributing, like fires elsewhere, because the model underestimates observed concentrations. The combined use of remote sensing, surface measurements, and transport modelling proved effective in describing the episode and distinguishing its causes.

In recent years, the pan-Arctic region has experienced increasingly extreme fire seasons. Fires in the northern high latitudes are driven by current and future climate change, lightning, fuel conditions, and human activity. In this context, conceptualizing and parameterizing current and future Arctic fire regimes will be important for fire and land management as well as understanding current and predicting future fire emissions. The objectives of this review were driven by policy questions identified by the Arctic Monitoring and Assessment Programme (AMAP) Working Group and posed to its Expert Group on Short-Lived Climate Forcers. This review synthesizes current understanding of the changing Arctic and boreal fire regimes, particularly as fire activity and its response to future climate change in the pan-Arctic have consequences for Arctic Council states aiming to mitigate and adapt to climate change in the north. The conclusions from our synthesis are the following. (1) Current and future Arctic fires, and the adjacent boreal region, are driven by natural (i.e. lightning) and human-caused ignition sources, including fires caused by timber and energy extraction, prescribed burning for landscape management, and tourism activities. Little is published in the scientific literature about cultural burning by Indigenous populations across the pan-Arctic, and questions remain on the source of ignitions above 70∘ N in Arctic Russia. (2) Climate change is expected to make Arctic fires more likely by increasing the likelihood of extreme fire weather, increased lightning activity, and drier vegetative and ground fuel conditions. (3) To some extent, shifting agricultural land use and forest transitions from forest–steppe to steppe, tundra to taiga, and coniferous to deciduous in a warmer climate may increase and decrease open biomass burning, depending on land use in addition to climate-driven biome shifts. However, at the country and landscape scales, these relationships are not well established. (4) Current black carbon and PM2.5 emissions from wildfires above 50 and 65∘ N are larger than emissions from the anthropogenic sectors of residential combustion, transportation, and flaring. Wildfire emissions have increased from 2010 to 2020, particularly above 60∘ N, with 56 % of black carbon emissions above 65∘ N in 2020 attributed to open biomass burning – indicating how extreme the 2020 wildfire season was and how severe future Arctic wildfire seasons can potentially be. (5) What works in the boreal zones to prevent and fight wildfires may not work in the Arctic. Fire management will need to adapt to a changing climate, economic development, the Indigenous and local communities, and fragile northern ecosystems, including permafrost and peatlands. (6) Factors contributing to the uncertainty of predicting and quantifying future Arctic fire regimes include underestimation of Arctic fires by satellite systems, lack of agreement between Earth observations and official statistics, and still needed refinements of location, conditions, and previous fire return intervals on peat and permafrost landscapes. This review highlights that much research is needed in order to understand the local and regional impacts of the changing Arctic fire regime on emissions and the global climate, ecosystems, and pan-Arctic communities.

We present 18 years (2001–2018) of aerosol measurements, including organic and elemental carbon (OC and EC), organic tracers (levoglucosan, arabitol, mannitol, trehalose, glucose, and 2-methyltetrols), trace elements, and ions, at the Birkenes Observatory (southern Norway) – a site representative of the northern European region. The OC/EC (2001–2018) and the levoglucosan (2008–2018) time series are the longest in Europe, with OC/EC available for the PM10, PM2.5 (fine), and PM10–2.5 (coarse) size fractions, providing the opportunity for a nearly 2-decade-long assessment. Using positive matrix factorization (PMF), we identify seven carbonaceous aerosol sources at Birkenes: mineral-dust-dominated aerosol (MIN), traffic/industry-like aerosol (TRA/IND), short-range-transported biogenic secondary organic aerosol (BSOASRT), primary biological aerosol particles (PBAP), biomass burning aerosol (BB), ammonium-nitrate-dominated aerosol (NH4NO3), and (one low carbon fraction) sea salt aerosol (SS). We observed significant (p), large decreases in EC in PM10 (−3.9 % yr−1) and PM2.5 (−4.2 % yr−1) and a smaller decline in levoglucosan (−2.8 % yr−1), suggesting that OC/EC from traffic and industry is decreasing, whereas the abatement of OC/EC from biomass burning has been slightly less successful. EC abatement with respect to anthropogenic sources is further supported by decreasing EC fractions in PM2.5 (−3.9 % yr−1) and PM10 (−4.5 % yr−1). PMF apportioned 72 % of EC to fossil fuel sources; this was further supported by PMF applied to absorption photometer data, which yielded a two-factor solution with a low aerosol Ångstrøm exponent (AAE = 0.93) fraction, assumed to be equivalent black carbon from fossil fuel combustion (eBCFF), contributing 78 % to eBC mass. The higher AAE fraction (AAE = 2.04) is likely eBC from BB (eBCBB). Source–receptor model calculations (FLEXPART) showed that continental Europe and western Russia were the main source regions of both elevated eBCBB and eBCFF. Dominating biogenic sources explain why there was no downward trend for OC. A relative increase in the OC fraction in PM2.5 (+3.2 % yr−1) and PM10 (+2.4 % yr−1) underscores the importance of biogenic sources at Birkenes (BSOA and PBAP), which were higher in the vegetative season and dominated both fine (53 %) and coarse (78 %) OC. Furthermore, 77 %–91 % of OC in PM2.5, PM10–2.5, and PM10 was attributed to biogenic sources in summer vs. 22 %–37 % in winter. The coarse fraction had the highest share of biogenic sources regardless of season and was dominated by PBAP, except in winter. Our results show a shift in the aerosol composition at Birkenes and, thus, also in the relative source contributions. The need for diverse offline and online carbonaceous aerosol speciation to understand carbonaceous aerosol sources, including their seasonal, annual, and long-term variability, has been demonstrated.

In recent years, ammonia emissions have been continuously increasing, being almost 4 times higher than in the 20th century. Although an important species, as its use as a fertilizer sustains human living, ammonia has major consequences for both humans and the environment because of its reactive gas-phase chemistry that makes it easily convertible to particles. Despite its pronounced importance, ammonia emissions are highly uncertain in most emission inventories. However, the great development of satellite remote sensing nowadays provides the opportunity for more targeted research on constraining ammonia emissions. Here, we used satellite measurements to calculate global ammonia emissions over the period 2008–2017. Then, the calculated ammonia emissions were fed to a chemistry transport model, and ammonia concentrations were simulated for the period 2008–2017. The simulated concentrations of ammonia were compared with ground measurements from Europe, North America and Southeastern Asia, as well as with satellite measurements. The satellite-constrained ammonia emissions represent global concentrations more accurately than state-of-the-art emissions. Calculated fluxes in the North China Plain were seen to be more increased after 2015, which is not due to emission changes but due to changes in sulfate emissions that resulted in less ammonia neutralization and hence in larger atmospheric loads. Emissions over Europe were also twice as much as those in traditional datasets with dominant sources being industrial and agricultural applications. Four hot-spot regions of high ammonia emissions were seen in North America, which are characterized by high agricultural activity, such as animal breeding, animal farms and agricultural practices. South America is dominated by ammonia emissions from biomass burning, which causes a strong seasonality. In Southeastern Asia, ammonia emissions from fertilizer plants in China, Pakistan, India and Indonesia are the most important, while a strong seasonality was observed with a spring and late summer peak due to rice and wheat cultivation. Measurements of ammonia surface concentrations were better reproduced with satellite-constrained emissions, such as measurements from CrIS (Cross-track Infrared Sounder).

Following the emergence of the severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) responsible for COVID-19 in December 2019 in Wuhan (China) and its spread to the rest of the world, the World Health Organization declared a global pandemic in March 2020. Without effective treatment in the initial pandemic phase, social distancing and mandatory quarantines were introduced as the only available preventative measure. In contrast to the detrimental societal impacts, air quality improved in all countries in which strict lockdowns were applied, due to lower pollutant emissions. Here we investigate the effects of the COVID-19 lockdowns in Europe on ambient black carbon (BC), which affects climate and damages health, using in situ observations from 17 European stations in a Bayesian inversion framework. BC emissions declined by 23 kt in Europe (20 % in Italy, 40 % in Germany, 34 % in Spain, 22 % in France) during lockdowns compared to the same period in the previous 5 years, which is partially attributed to COVID-19 measures. BC temporal variation in the countries enduring the most drastic restrictions showed the most distinct lockdown impacts. Increased particle light absorption in the beginning of the lockdown, confirmed by assimilated satellite and remote sensing data, suggests residential combustion was the dominant BC source. Accordingly, in central and Eastern Europe, which experienced lower than average temperatures, BC was elevated compared to the previous 5 years. Nevertheless, an average decrease of 11 % was seen for the whole of Europe compared to the start of the lockdown period, with the highest peaks in France (42 %), Germany (21 %), UK (13 %), Spain (11 %) and Italy (8 %). Such a decrease was not seen in the previous years, which also confirms the impact of COVID-19 on the European emissions of BC.

Plastic pollution is a critical concern across diverse ecosystems, yet most research has focused on terrestrial and aquatic transport, neglecting other mechanisms. Here the authors show that atmospheric transport is a major pathway for road plastic pollution over remote regions.

The Lagrangian particle dispersion model FLEXPART in its original version in the mid-1990s was designed for calculating the long-range and mesoscale dispersion of hazardous substances from point sources, such as those released after an accident in a nuclear power plant. Over the past decades, the model has evolved into a comprehensive tool for multi-scale atmospheric transport modeling and analysis and has attracted a global user community. Its application fields have been extended to a large range of atmospheric gases and aerosols, e.g., greenhouse gases, short-lived climate forcers like black carbon and volcanic ash, and it has also been used to study the atmospheric branch of the water cycle. Given suitable meteorological input data, it can be used for scales from dozens of meters to global. In particular, inverse modeling based on source–receptor relationships from FLEXPART has become widely used. In this paper, we present FLEXPART version 10.4, which works with meteorological input data from the European Centre for Medium-Range Weather Forecasts (ECMWF) Integrated Forecast System (IFS) and data from the United States National Centers of Environmental Prediction (NCEP) Global Forecast System (GFS). Since the last publication of a detailed FLEXPART description (version 6.2), the model has been improved in different aspects such as performance, physicochemical parameterizations, input/output formats, and available preprocessing and post-processing software. The model code has also been parallelized using the Message Passing Interface (MPI). We demonstrate that the model scales well up to using 256 processors, with a parallel efficiency greater than 75 % for up to 64 processes on multiple nodes in runs with very large numbers of particles. The deviation from 100 % efficiency is almost entirely due to the remaining nonparallelized parts of the code, suggesting large potential for further speedup. A new turbulence scheme for the convective boundary layer has been developed that considers the skewness in the vertical velocity distribution (updrafts and downdrafts) and vertical gradients in air density. FLEXPART is the only model available considering both effects, making it highly accurate for small-scale applications, e.g., to quantify dispersion in the vicinity of a point source. The wet deposition scheme for aerosols has been completely rewritten and a new, more detailed gravitational settling parameterization for aerosols has also been implemented. FLEXPART has had the option of running backward in time from atmospheric concentrations at receptor locations for many years, but this has now been extended to also work for deposition values and may become useful, for instance, for the interpretation of ice core measurements. To our knowledge, to date FLEXPART is the only model with that capability. Furthermore, the temporal variation and temperature dependence of chemical reactions with the OH radical have been included, allowing for more accurate simulations for species with intermediate lifetimes against the reaction with OH, such as ethane. Finally, user settings can now be specified in a more flexible namelist format, and output files can be produced in NetCDF format instead of FLEXPART's customary binary format. In this paper, we describe these new developments. Moreover, we present some tools for the preparation of the meteorological input data and for processing FLEXPART output data, and we briefly report on alternative FLEXPART versions.

Carbonaceous aerosol (total carbon, TCp) was source apportioned at nine European rural background sites, as part of the European Measurement and Evaluation Programme (EMEP) Intensive Measurement Periods in fall 2008 and winter/spring 2009. Five predefined fractions were apportioned based on ambient measurements: elemental and organic carbon, from combustion of biomass (ECbb and OCbb) and from fossil-fuel (ECff and OCff) sources, and remaining non-fossil organic carbon (OCrnf), dominated by natural sources.OCrnf made a larger contribution to TCp than anthropogenic sources (ECbb, OCbb, ECff, and OCff) at four out of nine sites in fall, reflecting the vegetative season, whereas anthropogenic sources dominated at all but one site in winter/spring. Biomass burning (OCbb + ECbb) was the major anthropogenic source at the central European sites in fall, whereas fossil-fuel (OCff + ECff) sources dominated at the southernmost and the two northernmost sites. Residential wood burning emissions explained 30 %–50 % of TCp at most sites in the first week of sampling in fall, showing that this source can be the dominant one, even outside the heating season. In winter/spring, biomass burning was the major anthropogenic source at all but two sites, reflecting increased residential wood burning emissions in the heating season. Fossil-fuel sources dominated EC at all sites in fall, whereas there was a shift towards biomass burning for the southernmost sites in winter/spring.Model calculations based on base-case emissions (mainly officially reported national emissions) strongly underpredicted observational derived levels of OCbb and ECbb outside Scandinavia. Emissions based on a consistent bottom-up inventory for residential wood burning (and including intermediate volatility compounds, IVOCs) improved model results compared to the base-case emissions, but modeled levels were still substantially underestimated compared to observational derived OCbb and ECbb levels at the southernmost sites.Our study shows that natural sources are a major contributor to carbonaceous aerosol in Europe, even in fall and in winter/spring, and that residential wood burning emissions are equally as large as or larger than that of fossil-fuel sources, depending on season and region. The poorly constrained residential wood burning emissions for large parts of Europe show the obvious need to improve emission inventories, with harmonization of emission factors between countries likely being the most important step to improve model calculations for biomass burning emissions, and European PM2.5 concentrations in general.

Highly unusual open fires burned in western Greenland between 31 July and 21 August 2017, after a period of warm, dry and sunny weather. The fires burned on peatlands that became vulnerable to fires by permafrost thawing. We used several satellite data sets to estimate that the total area burned was about 2345 ha. Based on assumptions of typical burn depths and emission factors for peat fires, we estimate that the fires consumed a fuel amount of about 117 kt C and emitted about 23.5 t of black carbon (BC) and 731 t of organic carbon (OC), including 141 t of brown carbon (BrC). We used a Lagrangian particle dispersion model to simulate the atmospheric transport and deposition of these species. We find that the smoke plumes were often pushed towards the Greenland ice sheet by westerly winds, and thus a large fraction of the emissions (30 %) was deposited on snow- or ice-covered surfaces. The calculated deposition was small compared to the deposition from global sources, but not entirely negligible. Analysis of aerosol optical depth data from three sites in western Greenland in August 2017 showed strong influence of forest fire plumes from Canada, but little impact of the Greenland fires. Nevertheless, CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) lidar data showed that our model captured the presence and structure of the plume from the Greenland fires. The albedo changes and instantaneous surface radiative forcing in Greenland due to the fire emissions were estimated with the SNICAR model and the uvspec model from the libRadtran radiative transfer software package. We estimate that the maximum albedo change due to the BC and BrC deposition was about 0.007, too small to be measured. The average instantaneous surface radiative forcing over Greenland at noon on 31 August was 0.03–0.04 W m−2, with locally occurring maxima of 0.63–0.77 W m−2 (depending on the studied scenario). The average value is up to an order of magnitude smaller than the radiative forcing from other sources. Overall, the fires burning in Greenland in the summer of 2017 had little impact on the Greenland ice sheet, causing a small extra radiative forcing. This was due to the – in a global context – still rather small size of the fires. However, the very large fraction of the emissions deposited on the Greenland ice sheet from these fires could contribute to accelerated melting of the Greenland ice sheet if these fires become several orders of magnitude larger under future climate.

Methane (CH4) is a powerful greenhouse gas. Its atmospheric mixing ratios have been increasing since 2005. Therefore, quantification of CH4 sources is essential for effective climate change mitigation. Here we report observations of the CH4 mixing ratios measured at the Zeppelin Observatory (Svalbard) in the Arctic and aboard the research vessel (RV) Helmer Hanssen over the Arctic Ocean from June 2014 to December 2016, as well as the long-term CH4 trend measured at the Zeppelin Observatory from 2001 to 2017. We investigated areas over the European Arctic Ocean to identify possible hotspot regions emitting CH4 from the ocean to the atmosphere, and used state-of-the-art modelling (FLEXPART) combined with updated emission inventories to identify CH4 sources. Furthermore, we collected air samples in the region as well as samples of gas hydrates, obtained from the sea floor, which we analysed using a new technique whereby hydrate gases are sampled directly into evacuated canisters. Using this new methodology, we evaluated the suitability of ethane and isotopic signatures (δ13C in CH4) as tracers for ocean-to-atmosphere CH4 emission. We found that the average methane / light hydrocarbon (ethane and propane) ratio is an order of magnitude higher for the same sediment samples using our new methodology compared to previously reported values, 2379.95 vs. 460.06, respectively. Meanwhile, we show that the mean atmospheric CH4 mixing ratio in the Arctic increased by 5.9±0.38 parts per billion by volume (ppb) per year (yr−1) from 2001 to 2017 and ∼8 pbb yr−1 since 2008, similar to the global trend of ∼ 7–8 ppb yr−1. Most large excursions from the baseline CH4 mixing ratio over the European Arctic Ocean are due to long-range transport from land-based sources, lending confidence to the present inventories for high-latitude CH4 emissions. However, we also identify a potential hotspot region with ocean–atmosphere CH4 flux north of Svalbard (80.4∘ N, 12.8∘ E) of up to 26 nmol m−2 s−1 from a large mixing ratio increase at the location of 30 ppb. Since this flux is consistent with previous constraints (both spatially and temporally), there is no evidence that the area of interest north of Svalbard is unique in the context of the wider Arctic. Rather, because the meteorology at the time of the observation was unique in the context of the measurement time series, we obtained over the short course of the episode measurements highly sensitive to emissions over an active seep site, without sensitivity to land-based emissions.

This paper presents the results of BC inversions at high northern latitudes (> 50° N) for the 2013–2015 period. A sensitivity analysis was performed to select the best representative species for BC and the best a priori emission dataset. The same model ensemble was used to assess the uncertainty of the a posteriori emissions of BC due to scavenging and removal and due to the use of different a priori emission inventory. A posteriori concentrations of BC simulated over Arctic regions were compared with independent observations from flight and ship campaigns showing, in all cases, smaller bias, which in turn witnesses the success of the inversion. The annual a posteriori emissions of BC at latitudes above 50° N were estimated as 560±171 kt yr−1, significantly smaller than in ECLIPSEv5 (745 kt yr−1), which was used and the a priori information in the inversions of BC. The average relative uncertainty of the inversions was estimated to be 30 %.A posteriori emissions of BC in North America are driven by anthropogenic sources, while biomass burning appeared to be less significant as it is also confirmed by satellite products. In northern Europe, a posteriori emissions were estimated to be half compared to the a priori ones, with the highest releases to be in megacities and due to biomass burning in eastern Europe. The largest emissions of BC in Siberia were calculated along the transect between Yekaterinsburg and Chelyabinsk. The optimised emissions of BC were high close to the gas flaring regions in Russia and in western Canada (Alberta), where numerous power and oil and gas production industries operate. Flaring emissions in Nenets–Komi oblast (Russia) were estimated to be much lower than in the a priori emissions, while in Khanty-Mansiysk (Russia) they remained the same after the inversions of BC. Increased emissions at the borders between Russia and Mongolia are probably due to biomass burning in villages along the Trans-Siberian Railway. The maximum BC emissions in high northern latitudes (> 50° N) were calculated for summer months due to biomass burning and they are controlled by seasonal variations in Europe and Asia, while North America showed a much smaller variability.

Climate predictions for the rapidly changing Arctic are highly uncertain, largely due to a poor understanding of the processes driving cloud properties. In particular, cloud fraction (CF) and cloud phase (CP) have major impacts on energy budgets, but are poorly represented in most models, often because of uncertainties in aerosol–cloud interactions. Here, we use over 10 million satellite observations coupled with aerosol transport model simulations to quantify large-scale microphysical effects of aerosols on CF and CP over the Arctic Ocean during polar night, when direct and semi-direct aerosol effects are minimal. Combustion aerosols over sea ice are associated with very large (∼ 10 W m−2) differences in longwave cloud radiative effects at the sea ice surface. However, co-varying meteorological changes on factors such as CF likely explain the majority of this signal. For example, combustion aerosols explain at most 40 % of the CF differences between the full dataset and the clean-condition subset, compared to between 57 % and 91 % of the differences that can be predicted by co-varying meteorology. After normalizing for meteorological regime, aerosol microphysical effects have small but significant impacts on CF, CP, and precipitation frequency on an Arctic-wide scale. These effects indicate that dominant aerosol–cloud microphysical mechanisms are related to the relative fraction of liquid-containing clouds, with implications for a warming Arctic.

Short-lived climate forcers have been proven important both for the climate and human health. In particular, black carbon (BC) is an important climate forcer both as an aerosol and when deposited on snow and ice surface because of its strong light absorption. This paper presents measurements of elemental carbon (EC; a measurement-based definition of BC) in snow collected from western Siberia and northwestern European Russia during 2014, 2015 and 2016. The Russian Arctic is of great interest to the scientific community due to the large uncertainty of emission sources there. We have determined the major contributing sources of BC in snow in western Siberia and northwestern European Russia using a Lagrangian atmospheric transport model. For the first time, we use a recently developed feature that calculates deposition in backward (so-called retroplume) simulations allowing estimation of the specific locations of sources that contribute to the deposited mass. EC concentrations in snow from western Siberia and northwestern European Russia were highly variable depending on the sampling location. Modelled BC and measured EC were moderately correlated (R = 0.53–0.83) and a systematic region-specific model underestimation was found. The model underestimated observations by 42 % (RMSE = 49 ng g−1) in 2014, 48 % (RMSE = 37 ng g−1) in 2015 and 27 % (RMSE = 43 ng g−1) in 2016. For EC sampled in northwestern European Russia the underestimation by the model was smaller (fractional bias, FB > −100 %). In this region, the major sources were transportation activities and domestic combustion in Finland. When sampling shifted to western Siberia, the model underestimation was more significant (FB

Since 1994, the In-service Aircraft for a Global Observing System (IAGOS) program has produced in situ measurements of the atmospheric composition during more than 51 000 commercial flights. In order to help analyze these observations and understand the processes driving the observed concentration distribution and variability, we developed the SOFT-IO tool to quantify source–receptor links for all measured data. Based on the FLEXPART particle dispersion model (Stohl et al., 2005), SOFT-IO simulates the contributions of anthropogenic and biomass burning emissions from the ECCAD emission inventory database for all locations and times corresponding to the measured carbon monoxide mixing ratios along each IAGOS flight. Contributions are simulated from emissions occurring during the last 20 days before an observation, separating individual contributions from the different source regions. The main goal is to supply added-value products to the IAGOS database by evincing the geographical origin and emission sources driving the CO enhancements observed in the troposphere and lower stratosphere. This requires a good match between observed and modeled CO enhancements. Indeed, SOFT-IO detects more than 95 % of the observed CO anomalies over most of the regions sampled by IAGOS in the troposphere. In the majority of cases, SOFT-IO simulates CO pollution plumes with biases lower than 10–15 ppbv. Differences between the model and observations are larger for very low or very high observed CO values. The added-value products will help in the understanding of the trace-gas distribution and seasonal variability. They are available in the IAGOS database via http://www.iagos.org. The SOFT-IO tool could also be applied to similar data sets of CO observations (e.g., ground-based measurements, satellite observations). SOFT-IO could also be used for statistical validation as well as for intercomparisons of emission inventories using large amounts of data.

Existing Lagrangian particle dispersion models are capable of establishing source–receptor relationships by running either forward or backward in time. For receptor-oriented studies such as interpretation of "point" measurement data, backward simulations can be computationally more efficient by several orders of magnitude. However, to date, the backward modelling capabilities have been limited to atmospheric concentrations or mixing ratios. In this paper, we extend the backward modelling technique to substances deposited at the Earth's surface by wet scavenging and dry deposition. This facilitates efficient calculation of emission sensitivities for deposition quantities at individual sites, which opens new application fields such as the comprehensive analysis of measured deposition quantities, or of deposition recorded in snow samples or ice cores. This could also include inverse modelling of emission sources based on such measurements. We have tested the new scheme as implemented in the Lagrangian particle dispersion model FLEXPART v10.2 by comparing results from forward and backward calculations. We also present an example application for black carbon concentrations recorded in Arctic snow.

Ice-nucleating particles (INPs) active at modest supercooling (e.g. −8 °C; INP−8) can transform clouds from liquid to mixed phase, even at very small number concentrations (−3). Over the course of 15 months, we found very similar patterns in weekly concentrations of INP−8 in PM10 (median = 1.7 m−3, maximum = 10.1 m−3) and weekly amounts of rainfall (median = 28 mm, maximum = 153 mm) at Birkenes, southern Norway. Most INP−8 were probably aerosolised locally by the impact of raindrops on plant, litter and soil surfaces. Major snowfall and heavy rain onto snow-covered ground were not mirrored by enhanced numbers of INP−8. Further, transport model calculations for large (> 4 m−3) and small (−3) numbers of INP−8 revealed that potential source regions likely to provide precipitation to southern Norway were associated with large numbers of INP−8. The proportion of land cover and land use type in potential source regions was similar for large and small numbers of INP−8. In PM2. 5 we found consistently about half as many INP−8 as in PM10. From mid-May to mid-September, INP−8 correlated positively with the fungal spore markers arabitol and mannitol, suggesting that some fraction of INP−8 during that period may consist of fungal spores. In the future, warmer winters with more rain instead of snow may enhance airborne concentrations of INP−8 during the cold season in southern Norway and in other regions with a similar climate.

Icelandic dust sources are known to be highly active, yet there exist few model simulations of Icelandic dust that could be used to assess its impacts on the environment. We here present estimates of dust emission and transport in Iceland over 27 years (1990–2016) based on FLEXDUST and FLEXPART simulations and meteorological re-analysis data. Simulations for the year 2012 based on high-resolution operational meteorological analyses are used for model evaluation based on PM2. 5 and PM10 observations in Iceland. For stations in Reykjavik, we find that the spring period is well predicted by the model, while dust events in late fall and early winter are overpredicted. Six years of dust concentrations observed at Stórhöfði (Heimaey) show that the model predicts concentrations of the same order of magnitude as observations and timing of modelled and observed dust peaks agrees well. Average annual dust emission is 4.3 ± 0.8 Tg during the 27 years of simulation. Fifty percent of all dust from Iceland is on average emitted in just 25 days of the year, demonstrating the importance of a few strong events for annual total dust emissions. Annual dust emission as well as transport patterns correlate only weakly to the North Atlantic Oscillation. Deposition amounts in remote regions (Svalbard and Greenland) vary from year to year. Only limited dust amounts reach the upper Greenland Ice Sheet, but considerable dust amounts are deposited on Icelandic glaciers and can impact melt rates there. Approximately 34 % of the annual dust emission is deposited in Iceland itself. Most dust (58 %), however, is deposited in the ocean and may strongly influence marine ecosystems.

Aerosol indirect effects have potentially large impacts on the Arctic Ocean surface energy budget, but model estimates of regional-scale aerosol indirect effects are highly uncertain and poorly validated by observations. Here we demonstrate a new way to quantitatively estimate aerosol indirect effects on a regional scale from remote sensing observations. In this study, we focus on nighttime, optically thin, predominantly liquid clouds. The method is based on differences in cloud physical and microphysical characteristics in carefully selected clean, average, and aerosol-impacted conditions. The cloud subset of focus covers just ∼ 5 % of cloudy Arctic Ocean regions, warming the Arctic Ocean surface by ∼ 1–1.4 W m−2 regionally during polar night. However, within this cloud subset, aerosol and cloud conditions can be determined with high confidence using CALIPSO and CloudSat data and model output. This cloud subset is generally susceptible to aerosols, with a polar nighttime estimated maximum regionally integrated indirect cooling effect of ∼ −0.11 W m−2 at the Arctic sea ice surface (∼ 8 % of the clean background cloud effect), excluding cloud fraction changes. Aerosol presence is related to reduced precipitation, cloud thickness, and radar reflectivity, and in some cases, an increased likelihood of cloud presence in the liquid phase. These observations are inconsistent with a glaciation indirect effect and are consistent with either a deactivation effect or less-efficient secondary ice formation related to smaller liquid cloud droplets. However, this cloud subset shows large differences in surface and meteorological forcing in shallow and higher-altitude clouds and between sea ice and open-ocean regions. For example, optically thin, predominantly liquid clouds are much more likely to overlay another cloud over the open ocean, which may reduce aerosol indirect effects on the surface. Also, shallow clouds over open ocean do not appear to respond to aerosols as strongly as clouds over stratified sea ice environments, indicating a larger influence of meteorological forcing over aerosol microphysics in these types of clouds over the rapidly changing Arctic Ocean.

A new, more physically based wet removal scheme for aerosols has been implemented in the Lagrangian particle dispersion model FLEXPART. It uses three-dimensional cloud water fields from the European Centre for Medium-Range Weather Forecasts (ECMWF) to determine cloud extent and distinguishes between in-cloud and below-cloud scavenging. The new in-cloud nucleation scavenging depends on cloud water phase (liquid, ice or mixed-phase), based on the aerosol's prescribed efficiency to serve as ice crystal nuclei and liquid water nuclei, respectively. The impaction scavenging scheme now parameterizes below-cloud removal as a function of aerosol particle size and precipitation type (snow or rain) and intensity.Sensitivity tests with the new scavenging scheme and comparisons with observational data were conducted for three distinct types of primary aerosols, which pose different challenges for modeling wet scavenging due to their differences in solubility, volatility and size distribution: (1) 137Cs released during the Fukushima nuclear accident attached mainly to highly soluble sulphate aerosol particles, (2) black carbon (BC) aerosol particles, and (3) mineral dust. Calculated e-folding lifetimes of accumulation mode aerosols for these three aerosol types were 11.7, 16.0, and 31.6 days respectively, when well mixed in the atmosphere. These are longer lifetimes than those obtained by the previous removal schem, and, for mineral dust in particular, primarily result from very slow in-cloud removal, which globally is the primary removal mechanism for these accumulation mode particles.Calculated e-folding lifetimes in FLEXPART also have a strong size dependence, with the longest lifetimes found for the accumulation-mode aerosols. For example, for dust particles emitted at the surface the lifetimes were 13.8 days for particles with 1 µm diameter and a few hours for 10 µm particles. A strong size dependence in below-cloud scavenging, combined with increased dry removal, is the primary reason for the shorter lifetimes of the larger particles. The most frequent removal is in-cloud scavenging (85 % of all scavenging events) but it occurs primarily in the free troposphere, while below-cloud removal is more frequent below 1000 m (52 % of all events) and can be important for the initial fate of species emitted at the surface, such as those examined here.For assumed realistic in-cloud removal efficiencies, both BC and sulphate have a slight overestimation of observed atmospheric concentrations (a factor of 1.6 and 1.2 respectively). However, this overestimation is largest close to the sources and thus appears more related to overestimated emissions rather than underestimated removal. The new aerosol wet removal scheme of FLEXPART incorporates more realistic information about clouds and aerosol properties and it compares better with both observed lifetimes and concentration than the old scheme.

In recent decades much attention has been given to the Arctic environment, where climate change is happening rapidly. Black carbon (BC) has been shown to be a major component of Arctic pollution that also affects the radiative balance. In the present study, we focused on how vegetation fires that occurred in northern Eurasia during the period of 2002–2013 influenced the budget of BC in the Arctic. For simulating the transport of fire emissions from northern Eurasia to the Arctic, we adopted BC fire emission estimates developed independently by GFED3 (Global Fire Emissions Database) and FEI-NE (Fire Emission Inventory – northern Eurasia). Both datasets were based on fire locations and burned areas detected by MODIS (Moderate resolution Imaging Spectroradiometer) instruments on NASA's (National Aeronautics and Space Administration) Terra and Aqua satellites. Anthropogenic sources of BC were adopted from the MACCity (Monitoring Atmospheric Composition and Climate and megacity Zoom for the Environment) emission inventory.During the 12-year period, an average area of 250 000 km2 yr−1 was burned in northern Eurasia (FEI-NE) and the global emissions of BC ranged between 8.0 and 9.5 Tg yr−1 (FEI-NE+MACCity). For the BC emitted in the Northern Hemisphere (based on FEI-NE+MACCity), about 70 % originated from anthropogenic sources and the rest from biomass burning (BB). Using the FEI-NE+MACCity inventory, we found that 102 ± 29 kt yr−1 BC was deposited in the Arctic (defined here as the area north of 67° N) during the 12 years simulated, which was twice as much as when using the MACCity inventory (56 ± 8 kt yr−1). The annual mass of BC deposited in the Arctic from all sources (FEI-NE in northern Eurasia, MACCity elsewhere) is significantly higher by about 37 % in 2009 (78 vs. 57 kt yr−1) to 181 % in 2012 (153 vs. 54 kt yr−1), compared to the BC deposited using just the MACCity emission inventory. Deposition of BC in the Arctic from BB sources in the Northern Hemisphere thus represents 68 % of the BC deposited from all BC sources (the remaining being due to anthropogenic sources). Northern Eurasian vegetation fires (FEI-NE) contributed 85 % (79–91 %) to the BC deposited over the Arctic from all BB sources in the Northern Hemisphere.We estimate that about 46 % of the BC deposited over the Arctic from vegetation fires in northern Eurasia originated from Siberia, 6 % from Kazakhstan, 5 % from Europe, and about 1 % from Mongolia. The remaining 42 % originated from other areas in northern Eurasia. About 42 % of the BC released from northern Eurasian vegetation fires was deposited over the Arctic (annual average: 17 %) during spring and summer.

The properties of low-level liquid clouds in the Arctic can be altered by long-range pollution transport to the region. Satellite, tracer transport model, and meteorological data sets are used here to determine a net aerosol–cloud interaction (ACInet) parameter that expresses the ratio of relative changes in cloud microphysical properties to relative variations in pollution concentrations while accounting for dry or wet scavenging of aerosols en route to the Arctic. For a period between 2008 and 2010, ACInet is calculated as a function of the cloud liquid water path, temperature, altitude, specific humidity, and lower tropospheric stability. For all data, ACInet averages 0.12 ± 0.02 for cloud-droplet effective radius and 0.16 ± 0.02 for cloud optical depth. It increases with specific humidity and lower tropospheric stability and is highest when pollution concentrations are low. Carefully controlling for meteorological conditions we find that the liquid water path of arctic clouds does not respond strongly to aerosols within pollution plumes. Or, not stratifying the data according to meteorological state can lead to artificially exaggerated calculations of the magnitude of the impacts of pollution on arctic clouds.

This paper presents a summary of the work done within the European Union's Seventh Framework Programme project ECLIPSE (Evaluating the Climate and Air Quality Impacts of Short-Lived Pollutants). ECLIPSE had a unique systematic concept for designing a realistic and effective mitigation scenario for short-lived climate pollutants (SLCPs; methane, aerosols and ozone, and their precursor species) and quantifying its climate and air quality impacts, and this paper presents the results in the context of this overarching strategy. The first step in ECLIPSE was to create a new emission inventory based on current legislation (CLE) for the recent past and until 2050. Substantial progress compared to previous work was made by including previously unaccounted types of sources such as flaring of gas associated with oil production, and wick lamps. These emission data were used for present-day reference simulations with four advanced Earth system models (ESMs) and six chemistry transport models (CTMs). The model simulations were compared with a variety of ground-based and satellite observational data sets from Asia, Europe and the Arctic. It was found that the models still underestimate the measured seasonality of aerosols in the Arctic but to a lesser extent than in previous studies. Problems likely related to the emissions were identified for northern Russia and India, in particular. To estimate the climate impacts of SLCPs, ECLIPSE followed two paths of research: the first path calculated radiative forcing (RF) values for a large matrix of SLCP species emissions, for different seasons and regions independently. Based on these RF calculations, the Global Temperature change Potential metric for a time horizon of 20 years (GTP20) was calculated for each SLCP emission type. This climate metric was then used in an integrated assessment model to identify all emission mitigation measures with a beneficial air quality and short-term (20-year) climate impact. These measures together defined a SLCP mitigation (MIT) scenario. Compared to CLE, the MIT scenario would reduce global methane (CH4) and black carbon (BC) emissions by about 50 and 80 %, respectively. For CH4, measures on shale gas production, waste management and coal mines were most important. For non-CH4 SLCPs, elimination of high-emitting vehicles and wick lamps, as well as reducing emissions from gas flaring, coal and biomass stoves, agricultural waste, solvents and diesel engines were most important. These measures lead to large reductions in calculated surface concentrations of ozone and particulate matter. We estimate that in the EU, the loss of statistical life expectancy due to air pollution was 7.5 months in 2010, which will be reduced to 5.2 months by 2030 in the CLE scenario. The MIT scenario would reduce this value by another 0.9 to 4.3 months. Substantially larger reductions due to the mitigation are found for China (1.8 months) and India (11–12 months). The climate metrics cannot fully quantify the climate response. Therefore, a second research path was taken. Transient climate ensemble simulations with the four ESMs were run for the CLE and MIT scenarios, to determine the climate impacts of the mitigation. In these simulations, the CLE scenario resulted in a surface temperature increase of 0.70 ± 0.14 K between the years 2006 and 2050. For the decade 2041–2050, the warming was reduced by 0.22 ± 0.07 K in the MIT scenario, and this result was in almost exact agreement with the response calculated based on the emission metrics (reduced warming of 0.22 ± 0.09 K). The metrics calculations suggest that non-CH4 SLCPs contribute ~ 22 % to this response and CH4 78 %. This could not be fully confirmed by the transient simulations, which attributed about 90 % of the temperature response to CH4 reductions. Attribution of the observed temperature response to non-CH4 SLCP emission reductions and BC specifically is hampered in the transient simulations by small forcing and co-emitted species of the emission basket chosen. Nevertheless, an important conclusion is that our mitigation basket as a whole would lead to clear benefits for both air quality and climate. The climate response from BC reductions in our study is smaller than reported previously, possibly because our study is one of the first to use fully coupled climate models, where unforced variability and sea ice responses cause relatively strong temperature fluctuations that may counteract (and, thus, mask) the impacts of small emission reductions. The temperature responses to the mitigation were generally stronger over the continents than over the oceans, and with a warming reduction of 0.44 K (0.39–0.49) K the largest over the Arctic. Our calculations suggest particularly beneficial climate responses in southern Europe, where surface warming was reduced by about 0.3 K and precipitation rates were increased by about 15 (6–21) mm yr−1 (more than 4 % of total precipitation) from spring to autumn. Thus, the mitigation could help to alleviate expected future drought and water shortages in the Mediterranean area. We also report other important results of the ECLIPSE project.

A detailed characterization of air quality in the megacity of Paris (France) during two 1-month intensive campaigns and from additional 1-year observations revealed that about 70 % of the urban background fine particulate matter (PM) is transported on average into the megacity from upwind regions. This dominant influence of regional sources was confirmed by in situ measurements during short intensive and longer-term campaigns, aerosol optical depth (AOD) measurements from ENVISAT, and modeling results from PMCAMx and CHIMERE chemistry transport models. While advection of sulfate is well documented for other megacities, there was surprisingly high contribution from long-range transport for both nitrate and organic aerosol. The origin of organic PM was investigated by comprehensive analysis of aerosol mass spectrometer (AMS), radiocarbon and tracer measurements during two intensive campaigns. Primary fossil fuel combustion emissions constituted less than 20 % in winter and 40 % in summer of carbonaceous fine PM, unexpectedly small for a megacity. Cooking activities and, during winter, residential wood burning are the major primary organic PM sources. This analysis suggests that the major part of secondary organic aerosol is of modern origin, i.e., from biogenic precursors and from wood burning. Black carbon concentrations are on the lower end of values encountered in megacities worldwide, but still represent an issue for air quality. These comparatively low air pollution levels are due to a combination of low emissions per inhabitant, flat terrain, and a meteorology that is in general not conducive to local pollution build-up. This revised picture of a megacity only being partially responsible for its own average and peak PM levels has important implications for air pollution regulation policies.

The concentrations of sulfate, black carbon (BC) and other aerosols in the Arctic are characterized by high values in late winter and spring (so-called Arctic Haze) and low values in summer. Models have long been struggling to capture this seasonality and especially the high concentrations associated with Arctic Haze. In this study, we evaluate sulfate and BC concentrations from eleven different models driven with the same emission inventory against a comprehensive pan-Arctic measurement data set over a time period of 2 years (2008–2009). The set of models consisted of one Lagrangian particle dispersion model, four chemistry transport models (CTMs), one atmospheric chemistry-weather forecast model and five chemistry climate models (CCMs), of which two were nudged to meteorological analyses and three were running freely. The measurement data set consisted of surface measurements of equivalent BC (eBC) from five stations (Alert, Barrow, Pallas, Tiksi and Zeppelin), elemental carbon (EC) from Station Nord and Alert and aircraft measurements of refractory BC (rBC) from six different campaigns. We find that the models generally captured the measured eBC or rBC and sulfate concentrations quite well, compared to previous comparisons. However, the aerosol seasonality at the surface is still too weak in most models. Concentrations of eBC and sulfate averaged over three surface sites are underestimated in winter/spring in all but one model (model means for January–March underestimated by 59 and 37 % for BC and sulfate, respectively), whereas concentrations in summer are overestimated in the model mean (by 88 and 44 % for July–September), but with overestimates as well as underestimates present in individual models. The most pronounced eBC underestimates, not included in the above multi-site average, are found for the station Tiksi in Siberia where the measured annual mean eBC concentration is 3 times higher than the average annual mean for all other stations. This suggests an underestimate of BC sources in Russia in the emission inventory used. Based on the campaign data, biomass burning was identified as another cause of the modeling problems. For sulfate, very large differences were found in the model ensemble, with an apparent anti-correlation between modeled surface concentrations and total atmospheric columns. There is a strong correlation between observed sulfate and eBC concentrations with consistent sulfate/eBC slopes found for all Arctic stations, indicating that the sources contributing to sulfate and BC are similar throughout the Arctic and that the aerosols are internally mixed and undergo similar removal. However, only three models reproduced this finding, whereas sulfate and BC are weakly correlated in the other models. Overall, no class of models (e.g., CTMs, CCMs) performed better than the others and differences are independent of model resolution.

Since the 1980s, emissions of SO2 and NOx (NO + NO2) from anthropogenic sources in the United States (US), Canada, and Europe have decreased significantly suggesting that the export of oxidized S and N compounds from surrounding continents to the atmosphere overlying the North Atlantic Ocean (NAO) has also decreased. The chemical compositions of aerosols and precipitation sampled daily on Bermuda (32.27° N, 64.87° W) from 1989 to 1997 and from 2006 to 2009 were evaluated to quantify the magnitudes, significance, and implications of associated tends in atmospheric composition. The chemical data were stratified based on FLEXPART (FLEXible PARTicle dispersion model) retroplumes into four discrete transport regimes: westerly flow from eastern North America (NEUS/SEUS); easterly trade-wind flow from northern Africa and the subtropical NAO (Africa); long, open-ocean, anticyclonic flow around the Bermuda High (Oceanic); and transitional flow from the relatively clean open ocean to the polluted eastern North America (North). Based on all data, annual average concentrations of non-sea-salt (nss) SO42– associated with aerosols and annual volume-weighted-average (VWA) concentrations in precipitation decreased significantly (by 22% and 49%, respectively) whereas annual VWA concentrations of NH4+ in precipitation increased significantly (by 70%). Corresponding trends in aerosol and precipitation NO3– and of aerosol NH4+ were insignificant. Nss SO42– in precipitation under NEUS/SEUS and Oceanic flow decreased significantly (61% each) whereas corresponding trends in particulate nss SO42– under both flow regimes were insignificant. Trends in precipitation composition were driven in part by decreasing emissions of SO2 over upwind continents and associated decreases in anthropogenic contributions to nss SO42– concentrations. Under NEUS/SEUS and Oceanic flow, the ratio of anthropogenic to biogenic contributions to nss SO42– in the column scavenged by precipitation were relatively greater than those in near surface aerosol, which implies that, for these flow regimes, precipitation is a better indicator of overall anthropogenic impacts on the lower troposphere. Particulate nss SO42– under African flow also decreased significantly (34%) whereas the corresponding decrease in nss SO42– associated with precipitation was insignificant. We infer that these trends were driven in part by reductions in the emissions and transport of oxidized S compounds from Europe. The lack of significant trends in NO3– associated with aerosols and precipitation under NEUS/SEUS flow is notable in light of the large decrease (37%) in NOx emissions in the US and Canada over the period of record. Rapid chemical processing of oxidized N in marine air contributed to this lack of correspondence. Decreasing ratios of nss SO42– to NH4+ and the significant decreasing trend in precipitation acidity (37%) indicate that the total amount of acidity in the multiphase gas–aerosol system in the western NAO troposphere decreased over the period of record. Decreasing aerosol acidities would have shifted the phase partitioning of total NH3 (NH3 + particulate NH4+ towards the gas phase thereby decreasing the atmospheric lifetime of total NH3 against wet plus dry deposition. The trend of increasing NH4+ in precipitation at Bermuda over the period of record suggests that NH3 emissions from surrounding continents also increased. Decreasing particulate nss SO42– in near-surface air under NEUS/SEUS flow over the period of record implies that the corresponding shortwave scattering and absorption by nss S and associated aerosols constituents also decreased. These changes in radiative transfer suggest a corresponding lower limit for net warming over the period in the range of 0.1–0.3 W m–2.

Levoglucosan, a highly specific tracer of particulate matter from biomass burning, has been used to study the influence of residential wood burning, agricultural waste burning and Boreal forest fire emissions on the Arctic atmosphere black carbon (BC) concentration. A one-year time series from March 2008 to March 2009 of levoglucosan has been established at the Zeppelin observatory in the European Arctic. Elevated concentrations of levoglucosan in winter (mean: 1.02 ng m−3) compared to summer (mean: 0.13 ng m−3) were observed, resembling the seasonal variation seen for e.g. sulfate and BC. The mean concentration in the winter period was 2–3 orders of magnitude lower than typical values reported for European urban areas in winter, and 1–2 orders of magnitude lower than European rural background concentrations. Episodes of elevated levoglucosan concentration lasting from 1 to 6 days were more frequent in winter than in summer and peak values were higher, exceeding 10 ng m−3 at the most. Concentrations of elemental carbon from biomass burning (ECbb) were obtained by combining measured concentrations of levoglucosan and emission ratios of levoglucosan and EC for wildfires/agricultural fires and for residential wood burning. Neglecting chemical degradation by OH provides minimum levoglucosan concentrations, corresponding to a mean ECbb concentration of 3.7 ± 1.2 ng m−3 in winter (October–April) and 0.8 ± 0.3 ng m−3 in summer (May–September), or 8.8 ± 4.5% of the measured equivalent black carbon (EBC) concentration in winter and 6.1 ± 3.4% in summer. When accounting for chemical degradation of levoglucosan by OH, an upper estimate of 31–45% of EBC could be attributed to ECbb* (ECbb adjusted for chemical degradation) in winter, whereas no reliable ( Calculations using the Lagrangian particle dispersion model FLEXPART show that the seasonal variation of the modeled ECbb (ECbb,m) concentration compared relatively well with observationally derived ECbb from agricultural fires/wildfires during summer, and residential wood burning in winter. The model overestimates by a factor of 2.2 in winter and 4.4 in summer when compared to the observationally derived mean ECbb concentration, which provides the minimum estimate, whereas it underestimates by a factor of 2.3–3.3 in winter and a factor of 4.5 in summer when compared to ECbb*, which provides the upper estimate. There are indications of too-low emissions of residential wood burning in northern Russia, a region of great importance with respect to observed concentrations of BC in the European Arctic.

Dichotomous aerosols (nominal super- and sub-μm-diameter size fractions) in sectored on-shore flow were sampled daily from July 2006 through June 2009, at the Tudor Hill Atmospheric Observatory (THAO) on the western coast of Bermuda (32.27° N, 64.87° W) and analyzed for major chemical and physical properties. FLEXPART retroplumes were calculated for each sampling period and aerosol properties were stratified accordingly based on transport from different regions. Transport from the northeastern United States (NEUS) was associated with significantly higher (factors of 2 to 3 based on median values) concentrations of bulk particulate non-sea-salt (nss) SO42-, NO3-, and NH4+ and associated scattering and absorption at 530 nm, relative to transport from Africa (AFR) and the oceanic background. These differences were driven primarily by higher values associated with the sub-μm size fraction under NEUS flow. We estimate that 75(±3)% of the NEUS nss SO42- was anthropogenic in origin, while only 25(±9)% of the AFR nss SO42- was anthropogenic. Integrating over all transport patterns, the contribution of anthropogenic sulfate has dropped 14.6% from the early 1990s. Bulk scattering was highly correlated with bulk nss SO42- in all flow regimes but the corresponding regression slopes varied significantly reflecting differential contributions to total scattering by associated aerosol components. Absorption by super-μm aerosol in transport from the NEUS versus AFR was similar although the super-μm aerosol size fraction accounted for a relatively greater contribution to total absorption in AFR flow. Significantly greater absorption Ångström exponents (AAEs) for AFR flow reflects the wavelength dependence of absorption by mineral aerosols; lower AAEs for NEUS flow is consistent with the dominance of absorption by combustion-derived aerosols. Higher AOD associated with transport from both the NEUS and AFR relative to oceanic background flow results in a top of atmosphere direct radiative forcing on the order of −1.6 to −2.5 W m−2, respectively, showing these aerosols drive cooling. The dominance of transport from the NEUS on an annual basis coupled with the corresponding decreases in anthropogenic nss SO42- aerosols since the early 1990s implies that emission reductions in the US account for a decline in atmospheric cooling over the western North Atlantic Ocean during this period.

Megacities are extreme examples of the continuously growing urbanization of the human population that pose (new) challenges to the environment and human health at a local scale. However, because of their size megacities also have larger-scale effects, and more research is needed to quantify their regional- and global-scale impacts. We performed a study of the characteristics of pollution plumes dispersing from a group of 36 of the world's megacities using the Lagrangian particle model FLEXPART and focusing on black carbon (BC) emissions during the years 2003–2005. BC was selected since it is representative of combustion-related emissions and has a significant role as a short-lived climate forcer. Based on the BC emissions two artificial tracers were modeled: a purely passive tracer and one subject to wet and dry deposition more closely resembling the behavior of a true aerosol. These tracers allowed us to investigate the role of deposition processes in determining the impact of megacities' pollutant plumes. The particles composing the plumes have been sampled in space and time. The time sampling allowed us to investigate the evolution of the plume from its release up to 48 days after emission and to generalize our results for any substance decaying with a timescale sufficiently shorter than the time window of 48 days. The physical characteristics of the time-averaged plume have been investigated, and this showed that, although local conditions are important, overall a city's latitude is the main factor influencing both the local and the regional-to-global dispersion of its pollution. We also repeated the calculations of some of the regional-pollution-potential metrics previously proposed by Lawrence et al. (2007), thus extending their results to a depositing scalar and retaining the evolution in time for all the plumes. Our results agreed well with their previous results despite being obtained using a totally different modeling framework. For the environmental impact on a global scale we focused on the export of mass from the megacities to the sensitive polar regions. We found that the sole city of Saint Petersburg contributes more to the lower-troposphere pollution and deposition in the Arctic than the whole ensemble of Asian megacities. In general this study showed that the pollution of urban origin in the lower troposphere of the Arctic is mainly generated by northern European sources. We also found that the deposition of the modeled artificial BC aerosol in the Antarctic due to megacities is comparable to the emissions of BC generated by local shipping activities. Finally multiplying population and ground level concentration maps, we found that the exposure of human population to megacity pollution occurs mainly inside the city boundaries, and this is especially true if deposition is accounted for. However, some exceptions exist (Beijing, Tianjin, Karachi) where the impact on population outside the city boundary is larger than that inside the city boundary.

Arctic haze is a seasonal phenomenon with high concentrations of accumulation-mode aerosols occurring in the Arctic in winter and early spring. Chemistry transport models and climate chemistry models struggle to reproduce this phenomenon, and this has recently prompted changes in aerosol removal schemes to remedy the modeling problems. In this paper, we show that shortcomings in current emission data sets are at least as important. We perform a 3 yr model simulation of black carbon (BC) with the Lagrangian particle dispersion model FLEXPART. The model is driven with a new emission data set ("ECLIPSE emissions") which includes emissions from gas flaring. While gas flaring is estimated to contribute less than 3% of global BC emissions in this data set, flaring dominates the estimated BC emissions in the Arctic (north of 66° N). Putting these emissions into our model, we find that flaring contributes 42% to the annual mean BC surface concentrations in the Arctic. In March, flaring even accounts for 52% of all Arctic BC near the surface. Most of the flaring BC remains close to the surface in the Arctic, so that the flaring contribution to BC in the middle and upper troposphere is small. Another important factor determining simulated BC concentrations is the seasonal variation of BC emissions from residential combustion (often also called domestic combustion, which is used synonymously in this paper). We have calculated daily residential combustion emissions using the heating degree day (HDD) concept based on ambient air temperature and compare results from model simulations using emissions with daily, monthly and annual time resolution. In January, the Arctic-mean surface concentrations of BC due to residential combustion emissions are 150% higher when using daily emissions than when using annually constant emissions. While there are concentration reductions in summer, they are smaller than the winter increases, leading to a systematic increase of annual mean Arctic BC surface concentrations due to residential combustion by 68% when using daily emissions. A large part (93%) of this systematic increase can be captured also when using monthly emissions; the increase is compensated by a decreased BC burden at lower latitudes. In a comparison with BC measurements at six Arctic stations, we find that using daily-varying residential combustion emissions and introducing gas flaring emissions leads to large improvements of the simulated Arctic BC, both in terms of mean concentration levels and simulated seasonality. Case studies based on BC and carbon monoxide (CO) measurements from the Zeppelin observatory appear to confirm flaring as an important BC source that can produce pollution plumes in the Arctic with a high BC / CO enhancement ratio, as expected for this source type. BC measurements taken during a research ship cruise in the White, Barents and Kara seas north of the region with strong flaring emissions reveal very high concentrations of the order of 200–400 ng m−3. The model underestimates these concentrations substantially, which indicates that the flaring emissions (and probably also other emissions in northern Siberia) are rather under- than overestimated in our emission data set. Our results suggest that it may not be "vertical transport that is too strong or scavenging rates that are too low" and "opposite biases in these processes" in the Arctic and elsewhere in current aerosol models, as suggested in a recent review article (Bond et al., Bounding the role of black carbon in the climate system: a scientific assessment, J. Geophys. Res., 2013), but missing emission sources and lacking time resolution of the emission data that are causing opposite model biases in simulated BC concentrations in the Arctic and in the mid-latitudes.

In this study we have analyzed whether tourist cruise ships have an influence on measured sulfur dioxide (SO2), ozone (O3), Aitken mode particle and equivalent black carbon (EBC) concentrations at Ny Ålesund and Zeppelin Mountain on Svalbard in the Norwegian Arctic during summer. We separated the measurement data set into periods when ships were present and periods when ships were not present in the Kongsfjord area, according to a long-term record of the number of passengers visiting Ny Ålesund. We show that when ships with more than 50 passengers cruise in the Kongsfjord, measured daytime mean concentrations of 60 nm particles and EBC in summer show enhancements of 72 and 45%, respectively, relative to values when ships are not present. Even larger enhancements of 81 and 72% were found for stagnant conditions. In contrast, O3 concentrations were 5% lower on average and 7% lower under stagnant conditions, due to titration of O3 with the emitted nitric oxide (NO). The differences between the two data subsets are largest for the highest measured percentiles, while relatively small differences were found for the median concentrations, indicating that ship plumes are sampled relatively infrequently even when ships are present although they carry high pollutant concentrations. We estimate that the ships increased the total summer mean concentrations of SO2, 60 nm particles and EBC by 15, 18 and 11%, respectively. Our findings have two important implications. Firstly, even at such a remote Arctic observatory as Zeppelin, the measurements can be influenced by tourist ship emissions. Careful data screening is recommended before summertime Zeppelin data is used for data analysis or for comparison with global chemistry transport models. However, Zeppelin remains as one of the most valuable Arctic observatories, as most other Arctic observatories face even larger local pollution problems. Secondly, given landing statistics of tourist ships on Svalbard, it is suspected that large parts of the Svalbard archipelago are affected by cruise ship emissions. Thus, our results may be taken as a warning signal of future pan-Arctic conditions if Arctic shipping becomes more frequent and emission regulations are not strict enough.

A first long-term monitoring of selected persistent organic pollutants (POPs) in Antarctic air has been conducted at the Norwegian research station Troll (Dronning Maud Land). As target contaminants 32 PCB congeners, α- and γ-hexachlorocyclohexane (HCH), trans- and cis-chlordane, trans- and cis-nonachlor, p,p'- and o,p-DDT, DDD, DDE as well as hexachlorobenzene (HCB) were selected. The monitoring program with weekly samples taken during the period 2007–2010 was coordinated with the parallel program at the Norwegian Arctic monitoring site (Zeppelin mountain, Ny-Ålesund, Svalbard) in terms of priority compounds, sampling schedule as well as analytical methods. The POP concentration levels found in Antarctica were considerably lower than Arctic atmospheric background concentrations. Similar to observations for Arctic samples, HCB is the predominant POP compound, with levels of around 22 pg m−3 throughout the entire monitoring period. In general, the following concentration distribution was found for the Troll samples analyzed: HCB > Sum HCH > Sum PCB > Sum DDT > Sum chlordanes. Atmospheric long-range transport was identified as a major contamination source for POPs in Antarctic environments. Several long-range transport events with elevated levels of pesticides and/or compounds with industrial sources were identified based on retroplume calculations with a Lagrangian particle dispersion model (FLEXPART).

Aerosol hygroscopicity and refractory black carbon (rBC) properties were characterised during wintertime at a suburban site in Paris, one of the biggest European cities. Hygroscopic growth factor (GF) frequency distributions, characterised by distinct modes of more-hygroscopic background aerosol and non- or slightly hygroscopic aerosol of local (or regional) origin, revealed an increase of the relative contribution of the local sources compared to the background aerosol with decreasing particle size. BC-containing particles in Paris were mainly originating from fresh traffic emissions, whereas biomass burning only gave a minor contribution. The mass size distribution of the rBC cores peaked on average at an rBC core mass equivalent diameter of DMEV ~ 150 nm. The BC-containing particles were moderately coated (coating thickness Δcoat ~ 33 nm on average for rBC cores with DMEV = 180–280 nm) and an average mass absorption coefficient (MAC) of ~ 8.6 m2 g−1 at the wavelength λ = 880 nm was observed. Different time periods were selected to investigate the properties of BC-containing particles as a function of source and air mass type. The traffic emissions were found to be non-hygroscopic (GF ≈ 1.0), and essentially all particles with a dry mobility diameter (D0) larger than D0 = 110 nm contained an rBC core. rBC from traffic emissions was further observed to be uncoated within experimental uncertainty (Δcoat ~ 2 nm ± 10 nm), to have the smallest BC core sizes (maximum of the rBC core mass size distribution at DMEV ~ 100 nm) and to have the smallest MAC (~ 7.3 m2g−1 at λ = 880 nm). The biomass burning aerosol was slightly more hygroscopic than the traffic emissions (with a distinct slightly-hygroscopic mode peaking at GF ≈ 1.1–1.2). Furthermore, only a minor fraction (≤ 10%) of the slightly-hygroscopic particles with 1.1 ≤ GF ≤ 1.2 (and D0 = 265 nm) contained a detectable rBC core. The BC-containing particles from biomass burning were found to have a medium coating thickness as well as slightly larger mean rBC core sizes and MAC values compared to traffic emissions. The aerosol observed under the influence of aged air masses and air masses from Eastern Continental Europe was dominated by a~more-hygroscopic mode peaking at GF ≈ 1.6. Most particles (95%), in the more-hygroscopic mode at D0 = 265 nm, did not contain a detectable rBC core. A significant fraction of the BC-containing particles had a substantial coating with non-refractory aerosol components. MAC values of ~ 8.8 m2g−1 and ~ 8.3 m2g−1 at λ = 880 nm and mass mean rBC core diameters of 150 nm and 200 nm were observed for the aged and continental air mass types, respectively. The reason for the larger rBC core sizes compared to the fresh emissions – transport effects or a different rBC source – remains unclear. The dominant fraction of the BC-containing particles was found to have no or very little coating with non-refractory matter. The lack of coatings is consistent with the observation that the BC-containing particles are non- or slightly-hygroscopic, which makes them poor cloud condensation nuclei. It can therefore be expected that wet removal through nucleation scavenging is inefficient for fresh BC-containing particles in urban plumes. The mixing-state-specific cloud droplet activation behaviour of BC-containing particles including the effects of atmospheric aging processes should be considered in global simulations of atmospheric BC, as the wet removal efficiency remains a major source of uncertainty in its life-cycle.

Infrared satellite images are widely and successfully used to detect and follow atmospheric ash from erupting volcanoes. We describe a new radiative transfer model framework for the simulation of infrared radiances, which can be compared directly with satellite images. This can be helpful to get insight into the processes that affect the satellite retrievals. As input to the radiative transfer model, the distribution of ash is provided by simulations with the FLEXPART Lagrangian particle dispersion model, meteorological cloud information is adopted from the ECMWF analysis and the radiative transfer modelling is performed with the MYSTIC 3-D radiative transfer model. The model framework is used to study an episode during the Eyjafjallajökull eruption in 2010. It is found that to detect ash by the reverse absorption retrieval technique, accurate representation of the ash particle size distribution is required. Detailed investigation of individual pixels displays the radiative effects of various combinations of ash, liquid water and ice clouds. In order to be clearly detectable, the ash clouds need to be located at some distance above other clouds. If ash clouds are mixed with water clouds or are located only slightly above water clouds, detection of the ash becomes difficult. Simulations were also made using the so-called independent pixel approximation (IPA) instead of the fully 3-D radiative transfer modelling. In the two simulations, different clouds (or different parts of the clouds) or the ground are effectively emitting radiation towards the instrument, thus causing differences in the brightness temperature of up to ± 25 K. The presented model framework is useful for further studies of the processes that affect satellite imagery and may be used to test both new and existing ash retrieval algorithms.

During July 2009, a one-month measurement campaign was performed in the megacity of Paris. Amongst other measurement platforms, three stationary sites distributed over an area of 40 km in diameter in the greater Paris region enabled a detailed characterization of the aerosol particle and gas phase. Simulation results from the FLEXPART dispersion model were used to distinguish between different types of air masses sampled. It was found that the origin of air masses had a large influence on measured mass concentrations of the secondary species particulate sulphate, nitrate, ammonium, and oxygenated organic aerosol measured with the Aerodyne aerosol mass spectrometer in the submicron particle size range: particularly high concentrations of these species (about 4 μg m−3, 2 μg m−3, 2 μg m−3, and 7 μg m−3, respectively) were measured when aged material was advected from continental Europe, while for air masses originating from the Atlantic, much lower mass concentrations of these species were observed (about 1 μg m−3, 0.2 μg m−3, 0.4 μg m−3, and 1–3 μg m−3, respectively). For the primary emission tracers hydrocarbon-like organic aerosol, black carbon, and NOx it was found that apart from diurnal source strength variations and proximity to emission sources, local meteorology had the largest influence on measured concentrations, with higher wind speeds leading to larger dilution and therefore smaller measured concentrations. Also the shape of particle size distributions was affected by wind speed and air mass origin. Quasi-Lagrangian measurements performed under connected flow conditions between the three stationary sites were used to estimate the influence of the Paris emission plume onto its surroundings, which was found to be rather small. Rough estimates for the impact of the Paris emission plume on the suburban areas can be inferred from these measurements: Volume mixing ratios of 1–14 ppb of NOx, and upper limits for mass concentrations of about 1.5 μg m−3 of black carbon and of about 3 μg m−3 of hydrocarbon-like organic aerosol can be deduced which originate from both, local emissions and the overall Paris emission plume. The secondary aerosol particle phase species were found to be not significantly influenced by the Paris megacity, indicating their regional origin. The submicron aerosol mass concentrations of particulate sulphate, nitrate, and ammonium measured during time periods when air masses were advected from eastern central Europe were found to be similar to what has been found from other measurement campaigns in Paris and south-central France for this type of air mass origin, indicating that the results presented here are also more generally valid.

Abstract The Arctic is a sentinel of global change. This region is influenced by multiple physical and socio-economic drivers and feedbacks, impacting both the natural and human environment. Air pollution is one such driver that impacts Arctic climate change, ecosystems and health but significant uncertainties still surround quantification of these effects. Arctic air pollution includes harmful trace gases (e.g. tropospheric ozone) and particles (e.g. black carbon, sulphate) and toxic substances (e.g. polycyclic aromatic hydrocarbons) that can be transported to the Arctic from emission sources located far outside the region, or emitted within the Arctic from activities including shipping, power production, and other industrial activities. This paper qualitatively summarizes the complex science issues motivating the creation of a new international initiative, PACES (air Pollution in the Arctic: Climate, Environment and Societies). Approaches for coordinated, international and interdisciplinary research on this topic are described with the goal to improve predictive capability via new understanding about sources, processes, feedbacks and impacts of Arctic air pollution. Overarching research actions are outlined, in which we describe our recommendations for 1) the development of trans-disciplinary approaches combining social and economic research with investigation of the chemical and physical aspects of Arctic air pollution; 2) increasing the quality and quantity of observations in the Arctic using long-term monitoring and intensive field studies, both at the surface and throughout the troposphere; and 3) developing improved predictive capability across a range of spatial and temporal scales.

On 11 March 2011, an earthquake occurred about 130 km off the Pacific coast of Japan's main island Honshu, followed by a large tsunami. The resulting loss of electric power at the Fukushima Dai-ichi nuclear power plant developed into a disaster causing massive release of radioactivity into the atmosphere. In this study, we determine the emissions into the atmosphere of two isotopes, the noble gas xenon-133 (133Xe) and the aerosol-bound caesium-137 (137Cs), which have very different release characteristics as well as behavior in the atmosphere. To determine radionuclide emissions as a function of height and time until 20 April, we made a first guess of release rates based on fuel inventories and documented accident events at the site. This first guess was subsequently improved by inverse modeling, which combined it with the results of an atmospheric transport model, FLEXPART, and measurement data from several dozen stations in Japan, North America and other regions. We used both atmospheric activity concentration measurements as well as, for 137Cs, measurements of bulk deposition. Regarding 133Xe, we find a total release of 15.3 (uncertainty range 12.2–18.3) EBq, which is more than twice as high as the total release from Chernobyl and likely the largest radioactive noble gas release in history. The entire noble gas inventory of reactor units 1–3 was set free into the atmosphere between 11 and 15 March 2011. In fact, our release estimate is higher than the entire estimated 133Xe inventory of the Fukushima Dai-ichi nuclear power plant, which we explain with the decay of iodine-133 (half-life of 20.8 h) into 133Xe. There is strong evidence that the 133Xe release started before the first active venting was made, possibly indicating structural damage to reactor components and/or leaks due to overpressure which would have allowed early release of noble gases. For 137Cs, the inversion results give a total emission of 36.6 (20.1–53.1) PBq, or about 43% of the estimated Chernobyl emission. Our results indicate that 137Cs emissions peaked on 14–15 March but were generally high from 12 until 19 March, when they suddenly dropped by orders of magnitude at the time when spraying of water on the spent-fuel pool of unit 4 started. This indicates that emissions may not have originated only from the damaged reactor cores, but also from the spent-fuel pool of unit 4. This would also confirm that the spraying was an effective countermeasure. We explore the main dispersion and deposition patterns of the radioactive cloud, both regionally for Japan as well as for the entire Northern Hemisphere. While at first sight it seemed fortunate that westerly winds prevailed most of the time during the accident, a different picture emerges from our detailed analysis. Exactly during and following the period of the strongest 137Cs emissions on 14 and 15 March as well as after another period with strong emissions on 19 March, the radioactive plume was advected over Eastern Honshu Island, where precipitation deposited a large fraction of 137Cs on land surfaces. Radioactive clouds reached North America on 15 March and Europe on 22 March. By middle of April, 133Xe was fairly uniformly distributed in the middle latitudes of the entire Northern Hemisphere and was for the first time also measured in the Southern Hemisphere (Darwin station, Australia). In general, simulated and observed concentrations of 133Xe and 137Cs both at Japanese as well as at remote sites were in good quantitative agreement. Altogether, we estimate that 6.4 PBq of 137Cs, or 18% of the total fallout until 20 April, were deposited over Japanese land areas, while most of the rest fell over the North Pacific Ocean. Only 0.7 PBq, or 1.9% of the total fallout were deposited on land areas other than Japan.

An Aerosol Time-Of-Flight Mass Spectrometer (ATOFMS) was deployed to investigate the size-resolved chemical composition of single particles at an urban background site in Paris, France, as part of the MEGAPOLI winter campaign in January/February 2010. ATOFMS particle counts were scaled to match coincident Twin Differential Mobility Particle Sizer (TDMPS) data in order to generate hourly size-resolved mass concentrations for the single particle classes observed. The total scaled ATOFMS particle mass concentration in the size range 150–1067 nm was found to agree very well with the sum of concurrent High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and Multi-Angle Absorption Photometer (MAAP) mass concentration measurements of organic carbon (OC), inorganic ions and black carbon (BC) (R2 = 0.91). Clustering analysis of the ATOFMS single particle mass spectra allowed the separation of elemental carbon (EC) particles into four classes: (i) EC attributed to biomass burning (ECbiomass), (ii) EC attributed to traffic (ECtraffic), (iii) EC internally mixed with OC and ammonium sulfate (ECOCSOx), and (iv) EC internally mixed with OC and ammonium nitrate (ECOCNOx). Average hourly mass concentrations for EC-containing particles detected by the ATOFMS were found to agree reasonably well with semi-continuous quantitative thermal/optical EC and optical BC measurements (r2 = 0.61 and 0.65–0.68 respectively, n = 552). The EC particle mass assigned to fossil fuel and biomass burning sources also agreed reasonably well with BC mass fractions assigned to the same sources using seven-wavelength aethalometer data (r2 = 0.60 and 0.48, respectively, n = 568). Agreement between the ATOFMS and other instrumentation improved noticeably when a period influenced by significantly aged, internally mixed EC particles was removed from the intercomparison. 88% and 12% of EC particle mass was apportioned to fossil fuel and biomass burning respectively using the ATOFMS data compared with 85% and 15% respectively for BC estimated from the aethalometer model. On average, the mass size distribution for EC particles is bimodal; the smaller mode is attributed to locally emitted, mostly externally mixed EC particles, while the larger mode is dominated by aged, internally mixed ECOCNOx particles associated with continental transport events. Periods of continental influence were identified using the Lagrangian Particle Dispersion Model (LPDM) "FLEXPART". A consistent minimum between the two EC mass size modes was observed at approximately 400 nm for the measurement period. EC particles below this size are attributed to local emissions using chemical mixing state information and contribute 79% of the scaled ATOFMS EC particle mass, while particles above this size are attributed to continental transport events and contribute 21% of the EC particle mass. These results clearly demonstrate the potential benefit of monitoring size-resolved mass concentrations for the separation of local and continental EC emissions. Knowledge of the relative input of these emissions is essential for assessing the effectiveness of local abatement strategies.

The Civil Aircraft for the Regular Investigation of the Atmosphere Based on an Instrument Container (CARIBIC) project investigates physical and chemical processes in the Earth's atmosphere using a Lufthansa Airbus long-distance passenger aircraft. After the beginning of the explosive eruption of the Eyjafjallajökull volcano on Iceland on 14 April 2010, the first CARIBIC volcano-specific measurement flight was carried out over the Baltic Sea and Southern Sweden on 20 April. Two more flights followed: one over Ireland and the Irish Sea on 16 May and the other over the Norwegian Sea on 19 May 2010. During these three special mission flights the CARIBIC container proved its merits as a comprehensive flying laboratory. The elemental composition of particles collected over the Baltic Sea during the first flight (20 April) indicated the presence of volcanic ash. Over Northern Ireland and the Irish Sea (16 May), the DOAS system detected SO2 and BrO co-located with volcanic ash particles that increased the aerosol optical depth. Over the Norwegian Sea (19 May), the optical particle counter detected a strong increase of particles larger than 400 nm diameter in a region where ash clouds were predicted by aerosol dispersion models. Aerosol particle samples collected over the Irish Sea and the Norwegian Sea showed large relative enhancements of the elements silicon, iron, titanium and calcium. Non-methane hydrocarbon concentrations in whole air samples collected on 16 and 19 May 2010 showed a pattern of removal of several hydrocarbons that is typical for chlorine chemistry in the volcanic clouds. Comparisons of measured ash concentrations and simulations with the FLEXPART dispersion model demonstrate the difficulty of detailed volcanic ash dispersion modelling due to the large variability of the volcanic cloud sources, extent and patchiness as well as the thin ash layers formed in the volcanic clouds.

In the present study, natural and anthropogenic sources of particulate organic carbon (OCp) and elemental carbon (EC) have been quantified based on weekly filter samples of PM10 (particles with aerodynamic diameter 14C/12C ratio of total carbon (TC), have been used as input for source apportionment of the carbonaceous aerosol, whereas Latin Hypercube Sampling (LHS) was used to statistically treat the multitude of possible combinations resulting from this approach. The carbonaceous aerosol (here: TCp; i.e. particulate TC) was totally dominated by natural sources (69–86%), with biogenic secondary organic aerosol (BSOA) being the single most important source (48–57%). Interestingly, primary biological aerosol particles (PBAP) were the second most important source (20–32%). The anthropogenic contribution was mainly attributed to fossil fuel sources (OCff and ECff) (10–24%), whereas no more than 3–7% was explained by combustion of biomass (OCbb and ECbb) in this late summer campaign i.e. emissions from residential wood burning and/or wild/agricultural fires. Fossil fuel sources totally dominated the ambient EC loading, which accounted for 4–12% of TCp, whereas

The April–May, 2010 volcanic eruptions of Eyjafjallajökull, Iceland caused significant economic and social disruption in Europe whilst state of the art measurements and ash dispersion forecasts were heavily criticized by the aviation industry. Here we demonstrate for the first time that large improvements can be made in quantitative predictions of the fate of volcanic ash emissions, by using an inversion scheme that couples a priori source information and the output of a Lagrangian dispersion model with satellite data to estimate the volcanic ash source strength as a function of altitude and time. From the inversion, we obtain a total fine ash emission of the eruption of 8.3 ± 4.2 Tg for particles in the size range of 2.8–28 μm diameter. We evaluate the results of our model results with a posteriori ash emissions using independent ground-based, airborne and space-borne measurements both in case studies and statistically. Subsequently, we estimate the area over Europe affected by volcanic ash above certain concentration thresholds relevant for the aviation industry. We find that during three episodes in April and May, volcanic ash concentrations at some altitude in the atmosphere exceeded the limits for the "Normal" flying zone in up to 14 % (6–16 %), 2 % (1–3 %) and 7 % (4–11 %), respectively, of the European area. For a limit of 2 mg m−3 only two episodes with fractions of 1.5 % (0.2–2.8 %) and 0.9 % (0.1–1.6 %) occurred, while the current "No-Fly" zone criterion of 4 mg m−3 was rarely exceeded. Our results have important ramifications for determining air space closures and for real-time quantitative estimations of ash concentrations. Furthermore, the general nature of our method yields better constraints on the distribution and fate of volcanic ash in the Earth system.

Passive air samplers (PAS) were deployed at 86 European background sites during summer 2006 in order (i) to gain further insight into spatial patterns of persistent organic pollutants (POPs) in European background air and, (ii) to evaluate PAS as an alternative sampling technique under EMEP (Co-operative programme for monitoring and evaluation of the long-range transmissions of air pollutants in Europe). The samples were analyzed for selected PCBs, HCHs, DDTs, HCB, PAHs and chlordanes, and air concentrations were calculated on the basis of losses of performance reference compounds. Air concentrations of PCBs were generally lowest in more remote areas of northern Europe with elevated levels in more densely populated areas. γ-HCH was found at elevated levels in more central parts of Europe, whereas α-HCH, β-HCH and DDTs showed higher concentrations in the south-eastern part. There was no clear spatial pattern in the concentrations for PAHs, indicative of influence by local sources, rather than long range atmospheric transport (LRAT). HCB was evenly distributed across Europe, while the concentrations of chlordanes were typically low or non-detectable. A comparison of results obtained on the basis of PAS and active air sampling (AAS) illustrated that coordinated PAS campaigns have the potential serve as useful inter-comparison exercises within and across existing monitoring networks. The results also highlighted limitations of the current EMEP measurement network with respect to spatial coverage. We finally adopted an existing Lagrangian transport model (FLEXPART) as recently modified to incorporate key processes relevant for POPs to evaluate potential source regions affecting observed concentrations at selected sites. Using PCB-28 as an example, the model predicted concentrations which agreed within a factor of 3 with PAS measurements for all except 1 out of the 17 sites selected for this analysis.

As a part of the IPY project POLARCAT (Polar Study using Aircraft, Remote Sensing, Surface Measurements and Models, of Climate, Chemistry, Aerosols and Transport) and building on previous work (Hirdman et al., 2010), this paper studies the long-term trends of both atmospheric transport as well as equivalent black carbon (EBC) and sulphate for the three Arctic stations Alert, Barrow and Zeppelin. We find a general downward trend in the measured EBC concentrations at all three stations, with a decrease of −2.1±0.4 ng m−3 yr−1 (for the years 1989–2008) and −1.4±0.8 ng m−3 yr−1 (2002–2009) at Alert and Zeppelin respectively. The decrease at Barrow is, however, not statistically significant. The measured sulphate concentrations show a decreasing trend at Alert and Zeppelin of −15±3 ng m−3 yr−1 (1985–2006) and −1.3±1.2 ng m−3 yr−1 (1990–2008) respectively, while there is no trend detectable at Barrow. To reveal the contribution of different source regions on these trends, we used a cluster analysis of the output of the Lagrangian particle dispersion model FLEXPART run backward in time from the measurement stations. We have investigated to what extent variations in the atmospheric circulation, expressed as variations in the frequencies of the transport from four source regions with different emission rates, can explain the long-term trends in EBC and sulphate measured at these stations. We find that the long-term trend in the atmospheric circulation can only explain a minor fraction of the overall downward trend seen in the measurements of EBC (0.3–7.2%) and sulphate (0.3–5.3%) at the Arctic stations. The changes in emissions are dominant in explaining the trends. We find that the highest EBC and sulphate concentrations are associated with transport from Northern Eurasia and decreasing emissions in this region drive the downward trends. Northern Eurasia (cluster: NE, WNE and ENE) is the dominant emission source at all Arctic stations for both EBC and sulphate during most seasons. In wintertime, there are indications that the EBC emissions from the eastern parts of Northern Eurasia (ENE cluster) have increased over the last decade.

As a part of the IPY project POLARCAT (Polar Study using Aircraft, Remote Sensing, Surface Measurements and Models, of Climate Chemistry, Aerosols and Transport), this paper studies the sources of equivalent black carbon (EBC), sulphate, light-scattering aerosols and ozone measured at the Arctic stations Zeppelin, Alert, Barrow and Summit during the years 2000–2007. These species are important pollutants and climate forcing agents, and sulphate and EBC are main components of Arctic haze. To determine where these substances originate, the measurement data were combined with calculations using FLEXPART, a Lagrangian particle dispersion model. The climatology of atmospheric transport from surrounding regions on a twenty-day time scale modelled by FLEXPART shows that the stations Zeppelin, Alert and Barrow are highly sensitive to surface emissions in the Arctic and to emissions in high-latitude Eurasia in winter. Emission sensitivities over southern Asia and southern North America are small throughout the year. The high-altitude station Summit is an order of magnitude less sensitive to surface emissions in the Arctic whereas emissions in the southern parts of the Northern Hemisphere continents are more influential relative to the other stations. Our results show that for EBC and sulphate measured at Zeppelin, Alert and Barrow, northern Eurasia is the dominant source region. For sulphate, Eastern Europe and the metal smelting industry in Norilsk are particularly important. For EBC, boreal forest fires also contribute in summer. No evidence for any substantial contribution to EBC from sources in southern Asia is found. European air masses are associated with low ozone concentrations in winter due to titration by nitric oxides, but are associated with high ozone concentrations in summer due to photochemical ozone formation. There is also a strong influence of ozone depletion events in the Arctic boundary layer on measured ozone concentrations in spring and summer. These results will be useful for developing emission reduction strategies for the Arctic.