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Ozone depletion events (ODEs) occur every spring in the Arctic and have implications for the region's atmospheric oxidizing capacity, radiative balance, and mercury oxidation. Here, we comprehensively analyze ozone, ODEs, and their connection to meteorological and air mass history variables through statistical analyses, back trajectories, and machine learning (ML) at Villum Research Station, Station Nord, Greenland, from 1996 to 2019. We show that the ODE frequency and duration peak in May, followed by April and March, which is likely related to air masses spending more time over sea ice and increases in radiation from March to May. Back trajectories indicate that, as spring progresses, ODE air masses spend more time within the mixed layer, and the geographic origins move closer to Villum. Positive trends in ODE frequency and duration are observed during May (low confidence) and April (high confidence), respectively. Our analysis revealed that ODEs are favorable under sunny, calm conditions, with air masses arriving from northerly wind directions with sea ice contact. The ML model was able to reproduce the ODE occurrence and illuminated that radiation, time over sea ice, and temperature were important variables for modeling ODEs during March, April, and May, respectively. Several variables displayed threshold ranges for contributing to the positive prediction of ODEs vs. non-ODEs, notably temperature, radiation, wind direction, time spent over sea ice, and snow on land. Our ML methodology provides a framework for investigating and comparing the environmental drivers of ODEs between different Arctic sites and can be applied to other atmospheric phenomena (e.g., atmospheric-mercury depletion events).

Anthropogenic and natural emissions contribute to enhanced concentrations of aerosols in the Arctic winter and early spring, with most attention being paid to anthropogenic aerosols that contribute to so-called Arctic haze. Less-well-studied wintertime sea-spray aerosols (SSAs) under Arctic haze conditions are the focus of this study, since they can make an important contribution to wintertime Arctic aerosol abundances. Analysis of field campaign data shows evidence for enhanced local sources of SSAs, including marine organics at Utqiaġvik (formerly known as Barrow) in northern Alaska, United States, during winter 2014. Models tend to underestimate sub-micron SSAs and overestimate super-micron SSAs in the Arctic during winter, including the base version of the Weather Research Forecast coupled with Chemistry (WRF-Chem) model used here, which includes a widely used SSA source function based on Gong et al. (1997). Quasi-hemispheric simulations for winter 2014 including updated wind speed and sea-surface temperature (SST) SSA emission dependencies and sources of marine sea-salt organics and sea-salt sulfate lead to significantly improved model performance compared to observations at remote Arctic sites, notably for coarse-mode sodium and chloride, which are reduced. The improved model also simulates more realistic contributions of SSAs to inorganic aerosols at different sites, ranging from 20 %–93 % in the observations. Two-thirds of the improved model performance is from the inclusion of the dependence on SSTs. The simulation of nitrate aerosols is also improved due to less heterogeneous uptake of nitric acid on SSAs in the coarse mode and related increases in fine-mode nitrate. This highlights the importance of interactions between natural SSAs and inorganic anthropogenic aerosols that contribute to Arctic haze. Simulation of organic aerosols and the fraction of sea-salt sulfate are also improved compared to observations. However, the model underestimates episodes with elevated observed concentrations of SSA components and sub-micron non-sea-salt sulfate at some Arctic sites, notably at Utqiaġvik. Possible reasons are explored in higher-resolution runs over northern Alaska for periods corresponding to the Utqiaġvik field campaign in January and February 2014. The addition of a local source of sea-salt marine organics, based on the campaign data, increases modelled organic aerosols over northern Alaska. However, comparison with previous available data suggests that local natural sources from open leads, as well as local anthropogenic sources, are underestimated in the model. Missing local anthropogenic sources may also explain the low modelled (sub-micron) non-sea-salt sulfate at Utqiaġvik. The introduction of a higher wind speed dependence for sub-micron SSA emissions, also based on Arctic data, reduces biases in modelled sub-micron SSAs, while sea-ice fractions, including open leads, are shown to be an important factor controlling modelled super-micron, rather than sub-micron, SSAs over the north coast of Alaska. The regional results presented here show that modelled SSAs are more sensitive to wind speed dependence but that realistic modelling of sea-ice distributions is needed for the simulation of local SSAs, including marine organics. This study supports findings from the Utqiaġvik field campaign that open leads are the primary source of fresh and aged SSAs, including marine organic aerosols, during wintertime at Utqiaġvik; these findings do not suggest an influence from blowing snow and frost flowers. To improve model simulations of Arctic wintertime aerosols, new field data on processes that influence wintertime SSA production, in particular for fine-mode aerosols, are needed as is improved understanding about possible local anthropogenic sources.

Ice-nucleating particles (INPs) can initiate ice formation in clouds at temperatures above −38 ∘C through heterogeneous ice nucleation. As a result, INPs affect cloud microphysical and radiative properties, cloud lifetime, and precipitation behavior and thereby ultimately the Earth's climate. Yet, little is known regarding the sources, abundance and properties of INPs, especially in remote regions such as the Arctic. In this study, 2-year-long INP measurements (from July 2018 to September 2020) at Villum Research Station in northern Greenland are presented. A low-volume filter sampler was deployed to collect filter samples for offline INP analysis. An annual cycle of INP concentration (NINP) was observed, and the fraction of heat-labile INPs was found to be higher in months with low to no snow cover and lower in months when the surface was well covered in snow (> 0.8 m). Samples were categorized into three different types based only on the slope of their INP spectra, namely into summer, winter and mix type. For each of the types a temperature-dependent INP parameterization was derived, clearly different depending on the time of the year. Winter and summer types occurred only during their respective seasons and were seen 60 % of the time. The mixed type occurred in the remaining 40 % of the time throughout the year. April, May and November were found to be transition months. A case study comparing April 2019 and April 2020 was performed. The month of April was selected because a significant difference in NINP was observed during these two periods, with clearly higher NINP in April 2020. In parallel to the observed differences in NINP, also a higher cloud-ice fraction was observed in satellite data for April 2020, compared to April 2019. NINP in the case study period revealed no clear dependency on either meteorological parameters or different surface types which were passed by the collected air masses. Overall, the results suggest that the coastal regions of Greenland were the main sources of INPs in April 2019 and 2020, most likely including both local terrestrial and marine sources.

Aerosol hygroscopic growth and cloud droplet formation influence the radiation transfer budget of the atmosphere and thereby the climate. In the Arctic, these aerosol properties may have a more pronounced effect on the climate compared to the midlatitudes. Hygroscopic growth and cloud condensation nuclei (CCN) concentrations of high Arctic aerosols were measured during two field studies in the spring and summer of 2016. The study site was the Villum Research Station (Villum) at Station Nord in the northeastern region of Greenland. Aerosol hygroscopic growth was measured with a hygroscopic tandem differential mobility analyzer (HTDMA) over a total of 23 d, and CCN concentrations were measured over a period of 95 d. Continuous particle number size distributions were recorded, facilitating calculations of aerosol CCN activation diameters and aerosol κ values. In spring, average CCN concentrations, at supersaturations (SSs) of 0.1 % to 0.3 %, ranged from 53.7 to 85.3 cm−3, with critical activation diameters ranging from 130.2 to 80.2 nm and κCCN ranging from 0.28–0.35. In summer, average CCN concentrations were 20.8 to 47.6 cm−3, while critical activation diameters and κCCN were from 137.1 to 76.7 nm and 0.23–0.35, respectively. Mean particle hygroscopic growth factors ranged from 1.60 to 1.75 at 90 % relative humidity in spring, while values between 1.47 and 1.67 were observed in summer depending on the initial dry size. Although the summer aerosol number size distributions were characterized by frequent new particle formation events, the CCN population at cloud-relevant supersaturations was determined by accumulation-mode aerosols.

Soot, or black carbon (BC), aerosol is a major climate forcer with severe health effects. The impacts depend strongly on particle number concentration, size and mixing state. This work reports on two field campaigns at nearby urban and rural sites, 65 km apart, in southern Sweden during late summer 2018. BC was measured using a single-particle soot photometer (SP2) and Aethalometers (AE33). Differences in BC concentrations between the sites are driven primarily by local traffic emissions. Equivalent and refractory BC mass concentrations at the urban site were on average a factor 2.2 and 2.5, with peaks during rush hour up to a factor ∼4, higher than the rural background levels. The number fraction of particles containing a soot core was significantly higher in the city. BC particles at the urban site were on average smaller by mass and had less coating owing to fresh traffic emissions. The organic components of the fresh traffic plumes were similar in mass spectral signature to hydrocarbon-like organic aerosol (HOA), commonly associated with traffic. Despite the intense local traffic (∼ 30 000 vehicles passing per day), PM1, including organic aerosol, was dominated by aged continental air masses even at the curbside site. The fraction of thickly coated particles at the urban site was highly correlated with the mass concentrations of all measured chemical species of PM1, consistent with aged, internally mixed aerosol. Trajectory analysis for the whole year showed that air masses arriving at the rural site from eastern Europe contained approximately double the amount of BC compared to air masses from western Europe. Furthermore, the largest regional emissions of BC transported to the rural site, from the Malmö–Copenhagen urban area, are discernible above background levels only when precipitation events are excluded. We show that continental Europe and not the Malmö–Copenhagen region is the major contributor to the background BC mass concentrations in southern Sweden.

The Arctic is a rapidly changing ecosystem, with complex ice–ocean–atmosphere feedbacks. An important process is new particle formation (NPF), from gas-phase precursors, which provides a climate forcing effect. NPF has been studied comprehensively at different sites in the Arctic, ranging from those in the High Arctic and those at Svalbard to those in the continental Arctic, but no harmonised analysis has been performed on all sites simultaneously, with no calculations of key NPF parameters available for some sites. Here, we analyse the formation and growth of new particles from six long-term ground-based stations in the Arctic (Alert, Villum, Tiksi, Zeppelin Mountain, Gruvebadet, and Utqiaġvik). Our analysis of particle formation and growth rates in addition to back-trajectory analysis shows a summertime maxima in the frequency of NPF and particle formation rate at all sites, although the mean frequency and particle formation rates themselves vary greatly between sites, with the highest at Svalbard and lowest in the High Arctic. The summertime growth rate, condensational sinks, and vapour source rates show a slight bias towards the southernmost sites, with vapour source rates varying by around an order of magnitude between the northernmost and southernmost sites. Air masses back-trajectories during NPF at these northernmost sites are associated with large areas of sea ice and snow, whereas events at Svalbard are associated with more sea ice and ocean regions. Events at the southernmost sites are associated with large areas of land and sea ice. These results emphasise how understanding the geographical variation in surface type across the Arctic is key to understanding secondary aerosol sources and providing a harmonised analysis of NPF across the Arctic.

As the third most important greenhouse gas (GHG) after carbon dioxide (CO2) and methane (CH4), tropospheric ozone (O3) is also an air pollutant causing damage to human health and ecosystems. This study brings together recent research on observations and modeling of tropospheric O3 in the Arctic, a rapidly warming and sensitive environment. At different locations in the Arctic, the observed surface O3 seasonal cycles are quite different. Coastal Arctic locations, for example, have a minimum in the springtime due to O3 depletion events resulting from surface bromine chemistry. In contrast, other Arctic locations have a maximum in the spring. The 12 state-of-the-art models used in this study lack the surface halogen chemistry needed to simulate coastal Arctic surface O3 depletion in the springtime; however, the multi-model median (MMM) has accurate seasonal cycles at non-coastal Arctic locations. There is a large amount of variability among models, which has been previously reported, and we show that there continues to be no convergence among models or improved accuracy in simulating tropospheric O3 and its precursor species. The MMM underestimates Arctic surface O3 by 5 % to 15 % depending on the location. The vertical distribution of tropospheric O3 is studied from recent ozonesonde measurements and the models. The models are highly variable, simulating free-tropospheric O3 within a range of ±50 % depending on the model and the altitude. The MMM performs best, within ±8 % for most locations and seasons. However, nearly all models overestimate O3 near the tropopause (∼300 hPa or ∼8 km), likely due to ongoing issues with underestimating the altitude of the tropopause and excessive downward transport of stratospheric O3 at high latitudes. For example, the MMM is biased high by about 20 % at Eureka. Observed and simulated O3 precursors (CO, NOx, and reservoir PAN) are evaluated throughout the troposphere. Models underestimate wintertime CO everywhere, likely due to a combination of underestimating CO emissions and possibly overestimating OH. Throughout the vertical profile (compared to aircraft measurements), the MMM underestimates both CO and NOx but overestimates PAN. Perhaps as a result of competing deficiencies, the MMM O3 matches the observed O3 reasonably well. Our findings suggest that despite model updates over the last decade, model results are as highly variable as ever and have not increased in accuracy for representing Arctic tropospheric O3.

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

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.

Even though the Arctic is remote, aerosol properties observed there are strongly influenced by anthropogenic emissions from outside the Arctic. This is particularly true for the so-called Arctic haze season (January through April). In summer (June through September), when atmospheric transport patterns change, and precipitation is more frequent, local Arctic sources, i.e., natural sources of aerosols and precursors, play an important role. Over the last few decades, significant reductions in anthropogenic emissions have taken place. At the same time a large body of literature shows evidence that the Arctic is undergoing fundamental environmental changes due to climate forcing, leading to enhanced emissions by natural processes that may impact aerosol properties. In this study, we analyze 9 aerosol chemical species and 4 particle optical properties from 10 Arctic observatories (Alert, Kevo, Pallas, Summit, Thule, Tiksi, Barrow/Utqiaġvik, Villum, and Gruvebadet and Zeppelin Observatory – both at Ny-Ålesund Research Station) to understand changes in anthropogenic and natural aerosol contributions. Variables include equivalent black carbon, particulate sulfate, nitrate, ammonium, methanesulfonic acid, sodium, iron, calcium and potassium, as well as scattering and absorption coefficients, single scattering albedo and scattering Ångström exponent. First, annual cycles are investigated, which despite anthropogenic emission reductions still show the Arctic haze phenomenon. Second, long-term trends are studied using the Mann–Kendall Theil–Sen slope method. We find in total 41 significant trends over full station records, i.e., spanning more than a decade, compared to 26 significant decadal trends. The majority of significantly declining trends is from anthropogenic tracers and occurred during the haze period, driven by emission changes between 1990 and 2000. For the summer period, no uniform picture of trends has emerged. Twenty-six percent of trends, i.e., 19 out of 73, are significant, and of those 5 are positive and 14 are negative. Negative trends include not only anthropogenic tracers such as equivalent black carbon at Kevo, but also natural indicators such as methanesulfonic acid and non-sea-salt calcium at Alert. Positive trends are observed for sulfate at Gruvebadet. No clear evidence of a significant change in the natural aerosol contribution can be observed yet. However, testing the sensitivity of the Mann–Kendall Theil–Sen method, we find that monotonic changes of around 5 % yr−1 in an aerosol property are needed to detect a significant trend within one decade. This highlights that long-term efforts well beyond a decade are needed to capture smaller changes. It is particularly important to understand the ongoing natural changes in the Arctic, where interannual variability can be high, such as with forest fire emissions and their influence on the aerosol population. To investigate the climate-change-induced influence on the aerosol population and the resulting climate feedback, long-term observations of tracers more specific to natural sources are needed, as well as of particle microphysical properties such as size distributions, which can be used to identify changes in particle populations which are not well captured by mass-oriented methods such as bulk chemical composition.

The global monitoring plan of the Minamata Convention on Mercury was established to generate long-term data necessary for evaluating the effectiveness of regulatory measures at a global scale. After 25 years of monitoring (since 1995), Mace Head is one of the atmospheric monitoring stations with the longest mercury record and has produced sufficient data for the analysis of temporal trends of total gaseous mercury (TGM) in Europe and the North Atlantic. Using concentration-weighted trajectories for atmospheric mercury measured at Mace Head as well as another five locations in Europe, Amderma, Andøya, Villum, Waldhof and Zeppelin, we identify the regional probabilistic source contribution factor and its changes for the period of 1996 to 2019. Temporal trends indicate that concentrations of mercury in the atmosphere in Europe and the North Atlantic have declined significantly over the past 25 years at a non-monotonic rate averaging 0.03 ngm-3yr-1. Concentrations of TGM at remote marine sites were shown to be affected by continental long-range transport, and evaluation of reanalysis back trajectories displays a significant decrease in TGM in continental air masses from Europe in the last 2 decades. In addition, using the relationship between mercury and other atmospheric trace gases that could serve as a source signature, we perform factorization regression analysis, based on positive rotatable factorization to solve probabilistic mass functions. We reconstructed atmospheric mercury concentration and assessed the contribution of the major natural and anthropogenic sources. The results reveal that the observed downward trend in the atmospheric mercury is mainly associated with a factor with a high load of long-lived anthropogenic species.

While much research has been devoted to the subject of gaseous elemental mercury (GEM) and gaseous oxidized mercury (GOM) in the Arctic spring during atmospheric mercury depletion events, few studies have examined the behavior of GOM in the High Arctic summer. GOM, once deposited and incorporated into the ecosystem, can pose a threat to human and wildlife health, though there remain large uncertainties regarding the transformation, deposition, and assimilation of mercury into the food web. Therefore, to further our understanding of the dynamics of GOM in the High Arctic during the late summer, we performed measurements of GEM and GOM, along with meteorological parameters and atmospheric constituents, and utilized modeled air mass history during two summer campaigns in 2019 and 2020 at Villum Research Station (Villum) in northeastern Greenland. Seven events of enhanced GOM concentrations were identified and investigated in greater detail. In general, the common factors associated with event periods at ground level were higher levels of radiation and lower H2O mixing ratios, accumulated precipitation, and relative humidity (RH), although none were connected with cold temperatures. Non-event periods at ground level each displayed a different pattern in one or more parameters when compared to event periods. Generally, air masses during event periods for both campaigns were colder and drier, arrived from higher altitudes, and spent more time above the mixed layer and less time in a cloud compared to non-events, although some events deviated from this general pattern. Non-event air masses displayed a different pattern in one or more parameters when compared to event periods, although they were generally warmer and wetter and arrived from lower altitudes with little radiation. Coarse-mode aerosols were hypothesized to provide the heterogenous surface for halogen propagation during some of the events, while for others the source is unknown. While these general patterns were observed for event and non-event periods, analysis of individual events showed more specific origins. Five of the seven events were associated with air masses that experienced similar conditions: transported from the cold, dry, and sunlit free troposphere. However, two events experienced contrasting conditions, with air masses being warm and wet with surface layer contact under little radiation. Two episodes of extremely high levels of NCoarse and BC, which appear to originate from flaring emissions in Russia, did not contribute to enhanced GOM levels. This work aims to provide a better understanding of the dynamics of GOM during the High Arctic summer.

The Arctic is warming 2 to 3 times faster than the global average, partly due to changes in short-lived climate forcers (SLCFs) including aerosols. In order to study the effects of atmospheric aerosols in this warming, recent past (1990–2014) and future (2015–2050) simulations have been carried out using the GISS-E2.1 Earth system model to study the aerosol burdens and their radiative and climate impacts over the Arctic (>60∘ N), using anthropogenic emissions from the Eclipse V6b and the Coupled Model Intercomparison Project Phase 6 (CMIP6) databases, while global annual mean greenhouse gas concentrations were prescribed and kept fixed in all simulations. Results showed that the simulations have underestimated observed surface aerosol levels, in particular black carbon (BC) and sulfate (SO42-), by more than 50 %, with the smallest biases calculated for the atmosphere-only simulations, where winds are nudged to reanalysis data. CMIP6 simulations performed slightly better in reproducing the observed surface aerosol concentrations and climate parameters, compared to the Eclipse simulations. In addition, simulations where atmosphere and ocean are fully coupled had slightly smaller biases in aerosol levels compared to atmosphere-only simulations without nudging. Arctic BC, organic aerosol (OA), and SO42- burdens decrease significantly in all simulations by 10 %–60 % following the reductions of 7 %–78 % in emission projections, with the Eclipse ensemble showing larger reductions in Arctic aerosol burdens compared to the CMIP6 ensemble. For the 2030–2050 period, the Eclipse ensemble simulated a radiative forcing due to aerosol–radiation interactions (RFARI) of -0.39±0.01 W m−2, which is −0.08 W m−2 larger than the 1990–2010 mean forcing (−0.32 W m−2), of which -0.24±0.01 W m−2 was attributed to the anthropogenic aerosols. The CMIP6 ensemble simulated a RFARI of −0.35 to −0.40 W m−2 for the same period, which is −0.01 to −0.06 W m−2 larger than the 1990–2010 mean forcing of −0.35 W m−2. The scenarios with little to no mitigation (worst-case scenarios) led to very small changes in the RFARI, while scenarios with medium to large emission mitigations led to increases in the negative RFARI, mainly due to the decrease in the positive BC forcing and the decrease in the negative SO42- forcing. The anthropogenic aerosols accounted for −0.24 to −0.26 W m−2 of the net RFARI in 2030–2050 period, in Eclipse and CMIP6 ensembles, respectively. Finally, all simulations showed an increase in the Arctic surface air temperatures throughout the simulation period. By 2050, surface air temperatures are projected to increase by 2.4 to 2.6 ∘C in the Eclipse ensemble and 1.9 to 2.6 ∘C in the CMIP6 ensemble, compared to the 1990–2010 mean. Overall, results show that even the scenarios with largest emission reductions leads to similar impact on the future Arctic surface air temperatures and sea-ice extent compared to scenarios with smaller emission reductions, implying reductions of greenhouse emissions are still necessary to mitigate climate change.

There are few long-term datasets of volatile organic compounds (VOCs) in the High Arctic. Furthermore, knowledge about their source regions remains lacking. To address this matter, we report a multiseason dataset of highly time-resolved VOC measurements in the High Arctic from April to October 2018. We have utilized a combination of measurement and modeling techniques to characterize the mixing ratios, temporal patterns, and sources of VOCs at the Villum Research Station at Station Nord in northeastern Greenland. Atmospheric VOCs were measured using proton-transfer-reaction time-of-flight mass spectrometry. Ten ions were selected for source apportionment with the positive matrix factorization (PMF) receptor model. A four-factor solution to the PMF model was deemed optimal. The factors identified were biomass burning, marine cryosphere, background, and Arctic haze. The biomass burning factor described the variation of acetonitrile and benzene and peaked during August and September. The marine cryosphere factor was comprised of carboxylic acids (formic, acetic, and C3H6O2) as well as dimethyl sulfide (DMS). This factor displayed peak contributions during periods of snow and sea ice melt. A potential source contribution function (PSCF) showed that the source regions for this factor were the coasts around southeastern and northeastern Greenland. The background factor was temporally ubiquitous, with a slight decrease in the summer. This factor was not driven by any individual chemical species. The Arctic haze factor was dominated by benzene with contributions from oxygenated VOCs. This factor exhibited a maximum in the spring and minima during the summer and autumn. This temporal pattern and species profile are indicative of anthropogenic sources in the midlatitudes. This study provides seasonal characteristics and sources of VOCs and can help elucidate the processes affecting the atmospheric chemistry and biogeochemical feedback mechanisms in the High Arctic.

Within the framework of the International Arctic Systems for Observing the Atmosphere (IASOA), we report a modelling-based study on surface ozone across the Arctic. We use surface ozone from six sites – Summit (Greenland), Pallas (Finland), Barrow (USA), Alert (Canada), Tiksi (Russia), and Villum Research Station (VRS) at Station Nord (North Greenland, Danish realm) – and ozone-sonde data from three Canadian sites: Resolute, Eureka, and Alert. Two global chemistry models – a global chemistry transport model (parallelised-Tropospheric Offline Model of Chemistry and Transport, p-TOMCAT) and a global chemistry climate model (United Kingdom Chemistry and Aerosol, UKCA) – are used for model data comparisons. Remotely sensed data of BrO from the GOME-2 satellite instrument and ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) at Eureka, Canada, are used for model validation. The observed climatology data show that spring surface ozone at coastal sites is heavily depleted, making ozone seasonality at Arctic coastal sites distinctly different from that at inland sites. Model simulations show that surface ozone can be greatly reduced by bromine chemistry. In April, bromine chemistry can cause a net ozone loss (monthly mean) of 10–20 ppbv, with almost half attributable to open-ocean-sourced bromine and the rest to sea-ice-sourced bromine. However, the open-ocean-sourced bromine, via sea spray bromide depletion, cannot by itself produce ozone depletion events (ODEs; defined as ozone volume mixing ratios, VMRs, < 10 ppbv). In contrast, sea-ice-sourced bromine, via sea salt aerosol (SSA) production from blowing snow, can produce ODEs even without bromine from sea spray, highlighting the importance of sea ice surface in polar boundary layer chemistry. Modelled total inorganic bromine (BrY) over the Arctic sea ice is sensitive to model configuration; e.g. under the same bromine loading, BrY in the Arctic spring boundary layer in the p-TOMCAT control run (i.e. with all bromine emissions) can be 2 times that in the UKCA control run. Despite the model differences, both model control runs can successfully reproduce large bromine explosion events (BEEs) and ODEs in polar spring. Model-integrated tropospheric-column BrO generally matches GOME-2 tropospheric columns within ∼ 50 % in UKCA and a factor of 2 in p-TOMCAT. The success of the models in reproducing both ODEs and BEEs in the Arctic indicates that the relevant parameterizations implemented in the models work reasonably well, which supports the proposed mechanism of SSA production and bromide release on sea ice. Given that sea ice is a large source of SSA and halogens, changes in sea ice type and extent in a warming climate will influence Arctic boundary layer chemistry, including the oxidation of atmospheric elemental mercury. Note that this work dose not necessary rule out other possibilities that may act as a source of reactive bromine from the sea ice zone.

Mercury is ubiquitous in the atmosphere, and atmospheric transport is an important source for this element in the Arctic. Measurements of gaseous elemental mercury (GEM) have been carried out at Villum Research Station (Villum) at Station Nord, situated in northern Greenland. The measurements cover the period 1999–2017, with a gap in the data for the period 2003–2008 (for a total of 11 years). The measurements were compared with model results from the Danish Eulerian Hemispheric Model (DEHM) that describes the contribution from direct anthropogenic transport, marine emissions and general background concentration. The percentage of time spent over different surfaces was calculated by back-trajectory analysis, and the reaction kinetics were determined by a comparison with ozone. The GEM measurements were analysed for trends, both seasonal and annual. The only significant trends found were negative ones for the winter and autumn months. Comparison of the measurements to simulations using the Danish Eulerian Hemispheric Model (DEHM) indicated that direct transport of anthropogenic emissions of mercury accounts for between 14 % and 17 % of the measured mercury. Analysis of the kinetics of the observed atmospheric mercury depletion events (AMDEs) confirms the results of a previous study at Villum of the competing reactions of GEM and ozone with Br, which suggests that the lifetime of GEM is about a month. However, a GEM lifetime of 12 months gave the best agreement between the model and measurements. The chemical lifetime is shorter, and thus, the apparent lifetime appears to be the result of deposition followed by reduction and re-emission; for this reason, the term “relaxation time” is preferred to “lifetime” for GEM. The relaxation time for GEM causes a delay between emission reductions and the effect on actual concentrations. No significant annual trend was found for the measured concentrations of GEM over the measurement period, despite emission reductions. This is interesting, and together with low direct transport of GEM to Villum as found by the DEHM model, it shows that the dynamics of GEM are very complex. Therefore, in the coming years, intensive measurement networks are needed to describe the global distribution of mercury in the environment as the use of models to predict future levels will still be highly uncertain. The situation is increasingly complex due to global changes that most likely will change the transport patterns of mercury, not only in the atmosphere but also between matrixes.

The role of polar regions is increasing in terms of megatrends such as globalization, new transport routes, demography, and the use of natural resources with consequent effects on regional and transported pollutant concentrations. We set up the ERA-PLANET Strand 4 project “iCUPE – integrative and Comprehensive Understanding on Polar Environments” to provide novel insights and observational data on global grand challenges with an Arctic focus. We utilize an integrated approach combining in situ observations, satellite remote sensing Earth observations (EOs), and multi-scale modeling to synthesize data from comprehensive long-term measurements, intensive campaigns, and satellites to deliver data products, metrics, and indicators to stakeholders concerning the environmental status, availability, and extraction of natural resources in the polar areas. The iCUPE work consists of thematic state-of-the-art research and the provision of novel data in atmospheric pollution, local sources and transboundary transport, the characterization of arctic surfaces and their changes, an assessment of the concentrations and impacts of heavy metals and persistent organic pollutants and their cycling, the quantification of emissions from natural resource extraction, and the validation and optimization of satellite Earth observation (EO) data streams. In this paper we introduce the iCUPE project and summarize initial results arising out of the integration of comprehensive in situ observations, satellite remote sensing, and multi-scale modeling in the Arctic context.

There are limited measurements of the chemical composition, abundance and sources of atmospheric particles in the High Arctic To address this, we report 93 d of soot particle aerosol mass spectrometer (SP-AMS) data collected from 20 February to 23 May 2015 at Villum Research Station (VRS) in northern Greenland (81∘36′ N). During this period, we observed the Arctic haze phenomenon with elevated PM1 concentrations ranging from an average of 2.3, 2.3 and 3.3 µg m−3 in February, March and April, respectively, to 1.2 µg m−3 in May. Particulate sulfate (SO42-) accounted for 66 % of the non-refractory PM1 with the highest concentration until the end of April and decreasing in May. The second most abundant species was organic aerosol (OA) (24 %). Both OA and PM1, estimated from the sum of all collected species, showed a marked decrease throughout May in accordance with the polar front moving north, together with changes in aerosol removal processes. The highest refractory black carbon (rBC) concentrations were found in the first month of the campaign, averaging 0.2 µg m−3. In March and April, rBC averaged 0.1 µg m−3 while decreasing to 0.02 µg m−3 in May. Positive matrix factorization (PMF) of the OA mass spectra yielded three factors: (1) a hydrocarbon-like organic aerosol (HOA) factor, which was dominated by primary aerosols and accounted for 12 % of OA mass, (2) an Arctic haze organic aerosol (AOA) factor and (3) a more oxygenated marine organic aerosol (MOA) factor. AOA dominated until mid-April (64 %–81 % of OA), while being nearly absent from the end of May and correlated significantly with SO42-, suggesting the main part of that factor is secondary OA. The MOA emerged late at the end of March, where it increased with solar radiation and reduced sea ice extent and dominated OA for the rest of the campaign until the end of May (24 %–74 % of OA), while AOA was nearly absent. The highest O∕C ratio (0.95) and S∕C ratio (0.011) was found for MOA. Our data support the current understanding that Arctic aerosols are highly influenced by secondary aerosol formation and receives an important contribution from marine emissions during Arctic spring in remote High Arctic areas. In view of a changing Arctic climate with changing sea-ice extent, biogenic processes and corresponding source strengths, highly time-resolved data are needed in order to elucidate the components dominating aerosol concentrations and enhance the understanding of the processes taking place.

Aerosols are an integral part of the Arctic climate system due to their direct interaction with radiation and indirect interaction through cloud formation. Understanding aerosol size distributions and their dynamics is crucial for the ability to predict these climate relevant effects. When of favourable size and composition, both long-range-transported – and locally formed particles – may serve as cloud condensation nuclei (CCN). Small changes of composition or size may have a large impact on the low CCN concentrations currently characteristic of the Arctic environment. We present a cluster analysis of particle size distributions (PSDs; size range 8–500 nm) simultaneously collected from three high Arctic sites during a 3-year period (2013–2015). Two sites are located in the Svalbard archipelago: Zeppelin research station (ZEP; 474 m above ground) and the nearby Gruvebadet Observatory (GRU; about 2 km distance from Zeppelin, 67 m above ground). The third site (Villum Research Station at Station Nord, VRS; 30 m above ground) is 600 km west-northwest of Zeppelin, at the tip of north-eastern Greenland. The GRU site is included in an inter-site comparison for the first time. K-means cluster analysis provided eight specific aerosol categories, further combined into broad PSD classes with similar characteristics, namely pristine low concentrations (12 %–14 % occurrence), new particle formation (16 %–32 %), Aitken (21 %–35 %) and accumulation (20 %–50 %). Confined for longer time periods by consolidated pack sea ice regions, the Greenland site GRU shows PSDs with lower ultrafine-mode aerosol concentrations during summer but higher accumulation-mode aerosol concentrations during winter, relative to the Svalbard sites. By association with chemical composition and cloud condensation nuclei properties, further conclusions can be derived. Three distinct types of accumulation-mode aerosol are observed during winter months. These are associated with sea spray (largest detectable sizes, >400 nm), Arctic haze (main mode at 150 nm) and aged accumulation-mode (main mode at 220 nm) aerosols. In contrast, locally produced particles, most likely of marine biogenic origin, exhibit size distributions dominated by the nucleation and Aitken mode during summer months. The obtained data and analysis point towards future studies, including apportioning the relative contribution of primary and secondary aerosol formation processes and elucidating anthropogenic aerosol dynamics and transport and removal processes across the Greenland Sea. In order to address important research questions in the Arctic on scales beyond a singular station or measurement events, it is imperative to continue strengthening international scientific cooperation.

Number concentrations of ice-nucleating particles (NINP) in the Arctic were derived from ground-based filter samples. Examined samples had been collected in Alert (Nunavut, northern Canadian archipelago on Ellesmere Island), Utqiaġvik, formerly known as Barrow (Alaska), Ny-Ålesund (Svalbard), and at the Villum Research Station (VRS; northern Greenland). For the former two stations, examined filters span a full yearly cycle. For VRS, 10 weekly samples, mostly from different months of one year, were included. Samples from Ny-Ålesund were collected during the months from March until September of one year. At all four stations, highest concentrations were found in the summer months from roughly June to September. For those stations with sufficient data coverage, an annual cycle can be seen. The spectra of NINP observed at the highest temperatures, i.e., those obtained for summer months, showed the presence of INPs that nucleate ice up to −5 ∘C. Although the nature of these highly ice-active INPs could not be determined in this study, it often has been described in the literature that ice activity observed at such high temperatures originates from the presence of ice-active material of biogenic origin. Spectra observed at the lowest temperatures, i.e., those derived for winter months, were on the lower end of the respective values from the literature on Arctic INPs or INPs from midlatitude continental sites, to which a comparison is presented herein. An analysis concerning the origin of INPs that were ice active at high temperatures was carried out using back trajectories and satellite information. Both terrestrial locations in the Arctic and the adjacent sea were found to be possible source areas for highly active INPs.

The Nordic Centre of Excellence CRAICC (Cryosphere–Atmosphere Interactions in a Changing Arctic Climate), funded by NordForsk in the years 2011–2016, is the largest joint Nordic research and innovation initiative to date, aiming to strengthen research and innovation regarding climate change issues in the Nordic region. CRAICC gathered more than 100 scientists from all Nordic countries in a virtual centre with the objectives of identifying and quantifying the major processes controlling Arctic warming and related feedback mechanisms, outlining strategies to mitigate Arctic warming, and developing Nordic Earth system modelling with a focus on short-lived climate forcers (SLCFs), including natural and anthropogenic aerosols. The outcome of CRAICC is reflected in more than 150 peer-reviewed scientific publications, most of which are in the CRAICC special issue of the journal Atmospheric Chemistry and Physics. This paper presents an overview of the main scientific topics investigated in the centre and provides the reader with a state-of-the-art comprehensive summary of what has been achieved in CRAICC with links to the particular publications for further detail. Faced with a vast amount of scientific discovery, we do not claim to completely summarize the results from CRAICC within this paper, but rather concentrate here on the main results which are related to feedback loops in climate change–cryosphere interactions that affect Arctic amplification.

Measurements of gaseous elemental mercury (GEM) fluxes over snow surfaces using a relaxed eddy accumulation (REA) system are carried out at the High Arctic site at the Villum Research Station, Station Nord, in North Greenland. Simultaneously, CO2 fluxes are determined using the eddy covariance (EC) technique. The REA system with dual inlets and dual analyzers is used to measure fluxes directly over the snow. The measurements were carried out from 23 April to 12 May during spring 2016, where atmospheric mercury depletion events (AMDEs) took place. The measurements showed a net emission of 8.9 ng m−2 min−1, with only a few minor episodes of net depositional fluxes, from a maximum deposition of 8.1 ng m−2 min−1 to a maximum emission of 179.2 ng m−2 min−1. The data support the theory that gaseous oxidized mercury (GOM) is deposited during AMDEs followed by formation of GEM on surface snow and is re-emitted as GEM shortly after the AMDEs. Furthermore, observation of the relation between GEM fluxes and atmospheric temperature suggests that GEM emission partly could be affected by surface heating. However, it is also clear that the GEM emissions are affected by many parameters.

The Arctic environment has an amplified response to global climatic change. It is sensitive to human activities that mostly take place elsewhere. For this study, a multi-year set of observed aerosol number size distributions in the diameter range of 10 to 500 nm from five sites around the Arctic Ocean (Alert, Villum Research Station – Station Nord, Zeppelin, Tiksi and Barrow) was assembled and analysed.A cluster analysis of the aerosol number size distributions revealed four distinct distributions. Together with Lagrangian air parcel back-trajectories, they were used to link the observed aerosol number size distributions with a variety of transport regimes. This analysis yields insight into aerosol dynamics, transport and removal processes, on both an intra- and an inter-monthly scale. For instance, the relative occurrence of aerosol number size distributions that indicate new particle formation (NPF) event is near zero during the dark months, increases gradually to ∼ 40 % from spring to summer, and then collapses in autumn. Also, the likelihood of Arctic haze aerosols is minimal in summer and peaks in April at all sites.The residence time of accumulation-mode particles in the Arctic troposphere is typically long enough to allow tracking them back to their source regions. Air flow that passes at low altitude over central Siberia and western Russia is associated with relatively high concentrations of accumulation-mode particles (Nacc) at all five sites – often above 150 cm−3. There are also indications of air descending into the Arctic boundary layer after transport from lower latitudes.The analysis of the back-trajectories together with the meteorological fields along them indicates that the main driver of the Arctic annual cycle of Nacc, on the larger scale, is when atmospheric transport covers the source regions for these particles in the 10-day period preceding the observations in the Arctic. The scavenging of these particles by precipitation is shown to be important on a regional scale and it is most active in summer. Cloud processing is an additional factor that enhances the Nacc annual cycle.There are some consistent differences between the sites that are beyond the year-to-year variability. They are the result of differences in the proximity to the aerosol source regions and to the Arctic Ocean sea-ice edge, as well as in the exposure to free-tropospheric air and in precipitation patterns – to mention a few. Hence, for most purposes, aerosol observations from a single Arctic site cannot represent the entire Arctic region. Therefore, the results presented here are a powerful observational benchmark for evaluation of detailed climate and air chemistry modelling studies of aerosols throughout the vast Arctic region.

This work presents an analysis of the physical properties of sub-micrometer aerosol particles measured at the high Arctic site Villum Research Station, Station Nord (VRS), northeast Greenland, between July 2010 and February 2013. The study focuses on particle number concentrations, particle number size distributions and the occurrence of new particle formation (NPF) events and their seasonality in the high Arctic, where observations and characterization of such aerosol particle properties and corresponding events are rare and understanding of related processes is lacking.A clear accumulation mode was observed during the darker months from October until mid-May, which became considerably more pronounced during the prominent Arctic haze months from March to mid-May. In contrast, nucleation- and Aitken-mode particles were predominantly observed during the summer months. Analysis of wind direction and wind speed indicated possible contributions of marine sources from the easterly side of the station to the observed summertime particle number concentrations, while southwesterly to westerly winds dominated during the darker months. NPF events lasting from hours to days were mostly observed from June until August, with fewer events observed during the months with less sunlight, i.e., March, April, September and October. The results tend to indicate that ozone (O3) might be weakly anti-correlated with particle number concentrations of the nucleation-mode range (10–30 nm) in almost half of the NPF events, while no positive correlation was observed. Calculations of air mass back trajectories using the Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model for the NPF event days suggested that the onset or interruption of events could possibly be explained by changes in air mass origin. A map of event occurrence probability was computed, indicating that southerly air masses from over the Greenland Sea were more likely linked to those events.

Long-term monitoring of data of ambient mercury (Hg) on a global scale to assess its emission, transport, atmospheric chemistry, and deposition processes is vital to understanding the impact of Hg pollution on the environment. The Global Mercury Observation System (GMOS) project was funded by the European Commission (http://www.gmos.eu) and started in November 2010 with the overall goal to develop a coordinated global observing system to monitor Hg on a global scale, including a large network of ground-based monitoring stations, ad hoc periodic oceanographic cruises and measurement flights in the lower and upper troposphere as well as in the lower stratosphere. To date, more than 40 ground-based monitoring sites constitute the global network covering many regions where little to no observational data were available before GMOS. This work presents atmospheric Hg concentrations recorded worldwide in the framework of the GMOS project (2010–2015), analyzing Hg measurement results in terms of temporal trends, seasonality and comparability within the network. Major findings highlighted in this paper include a clear gradient of Hg concentrations between the Northern and Southern hemispheres, confirming that the gradient observed is mostly driven by local and regional sources, which can be anthropogenic, natural or a combination of both.

Mercury (Hg) is a worldwide contaminant that can cause adverse health effects to wildlife and humans. While atmospheric modeling traces the link from emissions to deposition of Hg onto environmental surfaces, large uncertainties arise from our incomplete understanding of atmospheric processes (oxidation pathways, deposition, and re-emission). Atmospheric Hg reactivity is exacerbated in high latitudes and there is still much to be learned from polar regions in terms of atmospheric processes. This paper provides a synthesis of the atmospheric Hg monitoring data available in recent years (2011–2015) in the Arctic and in Antarctica along with a comparison of these observations with numerical simulations using four cutting-edge global models. The cycle of atmospheric Hg in the Arctic and in Antarctica presents both similarities and differences. Coastal sites in the two regions are both influenced by springtime atmospheric Hg depletion events and by summertime snowpack re-emission and oceanic evasion of Hg. The cycle of atmospheric Hg differs between the two regions primarily because of their different geography. While Arctic sites are significantly influenced by northern hemispheric Hg emissions especially in winter, coastal Antarctic sites are significantly influenced by the reactivity observed on the East Antarctic ice sheet due to katabatic winds. Based on the comparison of multi-model simulations with observations, this paper discusses whether the processes that affect atmospheric Hg seasonality and interannual variability are appropriately represented in the models and identifies research gaps in our understanding of the atmospheric Hg cycling in high latitudes.

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.

Semi-parameterized street canyon models, as e.g. the Operational Street Pollution Model (OSPM®), have been frequently applied for the last two decades to analyse levels and consequences of air pollution in streets. These models are popular due to their speed and low input requirements. One often-used simplification is the assumption that emissions are homogeneously distributed in the entire length and width of the street canyon. It is thus the aim of the present study to analyse the impact of this assumption by implementing an inhomogeneous emission geometry scheme in OSPM. The homogeneous and the inhomogeneous emission geometry schemes are validated against two real-world cases: Hornsgatan, Stockholm, a sloping street canyon; and Jagtvej, Copenhagen; where the morning rush hour has more traffic on one lane compared to the other. The two cases are supplemented with a theoretical calculation of the impact of street aspect (height / width) ratio and emission inhomogeneity on the concentrations resulting from inhomogeneous emissions. The results show an improved performance for the inhomogeneous emission geometry over the homogeneous emission geometry. Moreover, it is shown that the impact of inhomogeneous emissions is largest for near-parallel wind directions and for high aspect ratio canyons. The results from the real-world cases are however confounded by challenges estimating the emissions accurately.

Measurements of equivalent black carbon (EBC) in aerosols at the high Arctic field site Villum Research Station (VRS) at Station Nord in North Greenland showed a seasonal variation in EBC concentrations with a maximum in winter and spring at ground level. Average measured concentrations were about 0.067 ± 0.071 for the winter and 0.011 ± 0.009 for the summer period. These data were obtained using a multi-angle absorption photometer (MAAP). A similar seasonal pattern was found for sulfate concentrations with a maximum level during winter and spring analyzed by ion chromatography. Here, measured average concentrations were about 0.485 ± 0.397 for the winter and 0.112 ± 0.072 for the summer period. A correlation between EBC and sulfate concentrations was observed over the years 2011 to 2013 stating a correlation coefficient of R2 = 0.72. This finding gives the hint that most likely transport of primary emitted BC particles to the Arctic was accompanied by aging of the aerosols through condensational processes. BC and sulfate are known to have only partly similar sources with respect to their transport pathways when reaching the high Arctic. Aging processes may have led to the formation of secondary inorganic matter and further transport of BC particles as cloud processing and further washout of particles is less likely based on the typically observed transport patterns of air masses arriving at VRS. Additionally, concentrations of EC (elemental carbon) based on a thermo-optical method were determined and compared to EBC measurements. EBC measurements were generally higher, but a correlation between EC and EBC resulted in a correlation coefficient of R2 = 0.64. Model estimates of the climate forcing due to BC in the Arctic are based on contributions of long-range transported BC during spring and summer. The measured concentrations were here compared with model results obtained by the Danish Eulerian Hemispheric Model, DEHM. Good agreement between measured and modeled concentrations of both EBC/BC and sulfate was observed. Also, the correlation between BC and sulfate concentrations was confirmed based on the model results observed over the years 2011 to 2013 stating a correlation coefficient of R2 = 0.74. The dominant source is found to be combustion of fossil fuel with biomass burning as a minor, albeit significant source.

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.

Sources, composition and occurrence of secondary organic aerosols in the Arctic were investigated at Zeppelin Mountain, Svalbard, and Station Nord, northeastern Greenland, during the full annual cycle of 2008 and 2010, respectively. Speciation of organic acids, organosulfates and nitrooxy organosulfates – from both anthropogenic and biogenic precursors were in focus. A total of 11 organic acids (terpenylic acid, benzoic acid, phthalic acid, pinic acid, suberic acid, azelaic acid, adipic acid, pimelic acid, pinonic acid, diaterpenylic acid acetate and 3-methyl-1,2,3-butanetricarboxylic acid), 12 organosulfates and 1 nitrooxy organosulfate were identified in aerosol samples from the two sites using a high-performance liquid chromatograph (HPLC) coupled to a quadrupole Time-of-Flight mass spectrometer. At Station Nord, compound concentrations followed a distinct annual pattern, where high mean concentrations of organosulfates (47 ± 14 ng m−3) and organic acids (11.5 ± 4 ng m−3) were observed in January, February and March, contrary to considerably lower mean concentrations of organosulfates (2 ± 3 ng m−3) and organic acids (2.2 ± 1 ng m−3) observed during the rest of the year. At Zeppelin Mountain, organosulfate and organic acid concentrations remained relatively constant during most of the year at a mean concentration of 15 ± 4 ng m−3 and 3.9 ± 1 ng m−3, respectively. However during four weeks of spring, remarkably higher concentrations of total organosulfates (23–36 ng m−3) and total organic acids (7–10 ng m−3) were observed. Elevated organosulfate and organic acid concentrations coincided with the Arctic haze period at both stations, where northern Eurasia was identified as the main source region. Air mass transport from northern Eurasia to Zeppelin Mountain was associated with a 100% increase in the number of detected organosulfate species compared with periods of air mass transport from the Arctic Ocean, Scandinavia and Greenland. The results from this study suggested that the presence of organic acids and organosulfates at Station Nord was mainly due to long-range transport, whereas indications of local sources were found for some compounds at Zeppelin Mountain. Furthermore, organosulfates contributed significantly to organic matter throughout the year at Zeppelin Mountain (annual mean of 13 ± 8%) and during Arctic haze at Station Nord (7 ± 2%), suggesting organosulfates to be important compounds in Arctic aerosols.

Particles in the atmosphere are of concern due to their toxic properties and effects on climate. In coastal areas, ship emissions can be a significant anthropogenic source. In this study we investigated the contribution from ship emissions to the total particle number and mass concentrations at a remote location. We studied the particle number concentration (12 to 490 nm in diameter), the mass concentration (12 to 150 nm in diameter) and number and volume size distribution of aerosol particles in ship plumes for a period of 4.5 months at Høvsøre, a coastal site on the western coast of Jutland in Denmark. During episodes of western winds, the site is about 50 km downwind of a major shipping lane and the plumes are approximately 1 hour old when they arrive at the site. We have used a sliding percentile-based method for separating the plumes from the measured background values and to calculate the ship plume contribution to the total particle number and PM0.15 mass concentration (mass of particles below 150 nm in diameter, converted from volume assuming sphericity) at the site. The method is not limited to particle number or volume concentration, but can also be used for different chemical species in both particle and gas phase. The total number of analyzed ship plumes was 726, covering on average 19% of the time when air masses were arriving at the site over the shipping lane. During the periods when plumes were present, the particle concentration exceeded the background values on average by 790 cm−3 by number and 0.10 μg m−3 by mass. The corresponding daily average values were 170 cm−3 and 0.023 μg m−3, respectively. This means that the ship plumes contributed between 11 and 19% to the particle number concentration and between 9 and 18% to PM0.15 during days when air was arriving over the shipping lane. The estimated annual contribution from ship plumes, where all wind directions were included, was in the range of 5–8% in particle number concentration and 4–8% in PM0.15.

The knowledge of climate effects of atmospheric aerosols is associated with large uncertainty, and a better understanding of their physical and chemical properties is needed, especially in the Arctic environment. The objective of the present study is to improve our understanding of the processes affecting the composition of aerosols in the high Arctic. Therefore size-segregated aerosols were sampled at a high Arctic site, Station Nord (Northeast Greenland), in March 2009 using a Micro Orifice Uniform Deposit Impactor. The aerosol samples were extracted in order to analyse three water-soluble anions: chloride, nitrate and sulphate. The results are discussed based on possible chemical and physical transformations as well as transport patterns. The total concentrations of the ions at Station Nord were 53–507 ng m−3, 2–298 ng m−3 and 535–1087 ng m−3 for chloride (Cl−), nitrate (NO3−) and sulphate (SO42−), respectively. The aerosols in late winter/early spring, after polar sunrise, are found to be a mixture of long-range transported and regional to local originating aerosols. Fine particles, smaller than 1 μm, containing SO42−, Cl− and NO3−, are hypothesized to originate from long-range transport, where SO42− is by far the dominating anion accounting for 50–85% of the analyzed mass. The analysis suggests that Cl− and NO3− in coarser particles (> 1.5 μm) originate from local/regional sources. Under conditions where the air mass is transported over sea ice at high wind speeds, very coarse particles (> 18 μm) are observed, and it is hypothesized that frost flowers on the sea ice are a source of the very coarse nitrate particles.

In order to develop strategies for controlling and reducing Arctic air pollution, there is a need to understand the basic mechanisms for determining the fate of air pollution in the Arctic. Sources of atmospheric particles at Station Nord (81° 36' N, 16° 40' W) in North East Greenland were evaluated for a two-year period from March 2008 to February 2010. Source apportionment using Positive Matrix Factorization (PMF) and COnstrained Physical REceptor Model (COPREM) was based on measurements of black carbon, elements (Al, Si, S, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, Ga, As, Se, Br, Rb, Sr, Zr, Pb) and inorganic ions (SO2, SO42−, Na+, NH4+, NO3−, Cl2−. In general, source apportionment results by PMF and COPREM showed good agreement. Five sources adequately explained the measurements, which included a Marine and a Soil source of natural origin and three additional anthropogenic sources, which were all influenced by metal industries. One anthropogenic source was dominated by Zn of which air mass back trajectories using the Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model suggested a Canadian Arctic origin, despite certain influences from Southern and Eastern origins. Another anthropogenic source was characterised by high concentrations of Pb and As, which has been historically referred to as a Combustion source at Station Nord. The impacts of large-scale industry in Siberia, Russia were evident through high Cu concentrations in both the Combustion source and an additional Cu/Ni source. Br correlated well with the anthropogenic species S and Pb though the elements are unlikely to have a common origin. More likely, sulphuric acid aerosols serve as transport containers for Br species of marine origin. Of particular relevance to climate, sources of black carbon were identified to be mainly anthropogenic and most probably of Siberian origin (80–98%).

The pressure dependence of the relative photolysis rate of HCHO vs. HCDO has been investigated for the first time, using a photochemical reactor at the University of Copenhagen. The dissociation of HCHO vs. HCDO using a UVA lamp was measured at total bath gas pressures of 50, 200, 400, 600 and 1030 mbar. The products of formaldehyde photodissociation are either H2 + CO (molecular channel) or HCO + H (radical channel), and a photolysis lamp was chosen to emit light at wavelengths that greatly favor the molecular channel. The isotope effect in the dissociation, kHCHO/kHCDO, was found to depend strongly on pressure, varying from 1.1 + 0.15/−0.1 at 50 mbar to 1.75±0.10 at 1030 mbar. The results can be corrected for radical channel contribution to yield the kinetic isotope effect for the molecular channel; i.e. the KIE in the production of molecular hydrogen. This is done and the results at 1030 mbar are discussed in relation to previous studies at ambient pressure. In the atmosphere the relative importance of the two product channels changes with altitude as a result of changes in pressure and actinic flux. The study demonstrates that the δD of photochemical hydrogen produced from formaldehyde will increase substantially as pressure decreases.

It was discovered in 1995 that, during the spring time, unexpectedly low concentrations of gaseous elemental mercury (GEM) occurred in the Arctic air. This was surprising for a pollutant known to have a long residence time in the atmosphere; however conditions appeared to exist in the Arctic that promoted this depletion of mercury (Hg). This phenomenon is termed atmospheric mercury depletion events (AMDEs) and its discovery has revolutionized our understanding of the cycling of Hg in Polar Regions while stimulating a significant amount of research to understand its impact to this fragile ecosystem. Shortly after the discovery was made in Canada, AMDEs were confirmed to occur throughout the Arctic, sub-Artic and Antarctic coasts. It is now known that, through a series of photochemically initiated reactions involving halogens, GEM is converted to a more reactive species and is subsequently associated to particles in the air and/or deposited to the polar environment. AMDEs are a means by which Hg is transferred from the atmosphere to the environment that was previously unknown. In this article we review Hg research taken place in Polar Regions pertaining to AMDEs, the methods used to collect Hg in different environmental media, research results of the current understanding of AMDEs from field, laboratory and modeling work, how Hg cycles around the environment after AMDEs, gaps in our current knowledge and the future impacts that AMDEs may have on polar environments. The research presented has shown that while considerable improvements in methodology to measure Hg have been made but the main limitation remains knowing the speciation of Hg in the various media. The processes that drive AMDEs and how they occur are discussed. As well, the role that the snow pack and the sea ice play in the cycling of Hg is presented. It has been found that deposition of Hg from AMDEs occurs at marine coasts and not far inland and that a fraction of the deposited Hg does not remain in the same form in the snow. Kinetic studies undertaken have demonstrated that bromine is the major oxidant depleting Hg in the atmosphere. Modeling results demonstrate that there is a significant deposition of Hg to Polar Regions as a result of AMDEs. Models have also shown that Hg is readily transported to the Arctic from source regions, at times during springtime when this environment is actively transforming Hg from the atmosphere to the snow and ice surfaces. The presence of significant amounts of methyl Hg in snow in the Arctic surrounding AMDEs is important because this species is the link between the environment and impacts to wildlife and humans. Further, much work on methylation and demethylation processes has occurred but these processes are not yet fully understood. Recent changes in the climate and sea ice cover in Polar Regions are likely to have strong effects on the cycling of Hg in this environment; however more research is needed to understand Hg processes in order to formulate meaningful predictions of these changes.

A new 3-D mercury model has been developed within the Danish Arctic Monitoring and Assessment Programme (AMAP). The model is based on the Danish Eulerian Hemispheric Model, which in the original version has been used to study the transport of SO2, SO42- and Pb into the Arctic. It was developed for sulphur in 1990 and in 1999 also lead was included. For the current study a chemical scheme for mercury has been included and the model is now applied to the mercury transport problem. Some experiments with the formulation of the mercury chemistry during the Polar Sunrise are carried out in order to investigate the observed depletion. Some of the main conclusions of the work described in this paper are that atmospheric transport of mercury is a very important pathway into the Arctic and that mercury depletion in the Arctic troposphere during the Polar Sunrise contributes considerably to the deposition of mercury in the Arctic.

Abstract Pulmonary surfactant serves as a barrier to respiratory epithelium but can also regulate airway smooth muscle (ASM) tone. Surfactant (SF) relaxes contracted ASM, similar to β2‐agonists, anticholinergics, nitric oxide, and prostanoids. The exact mechanism of surfactant relaxation and whether surfactant relaxes hyperresponsive ASM remains unknown. Based on previous research, relaxation requires an intact epithelium and prostanoid synthesis. We sought to examine the mechanisms by which surfactant causes ASM relaxation. Organ bath measurements of isometric tension of ASM of guinea pigs in response to exogenous surfactant revealed that surfactant reduces tension of healthy and hyperresponsive tracheal tissue. The relaxant effect of surfactant was reduced if prostanoid synthesis was inhibited and/or if prostaglandin E2‐related EP2 receptors were antagonized. Atomic force microscopy revealed that human ASM cells stiffen during contraction and soften during relaxation. Surfactant softened ASM cells, similarly to the known bronchodilator prostaglandin E2 (PGE2) and the cell softening was abolished when EP4 receptors for PGE2 were antagonized. Elevated levels of PGE2 were found in cultures of normal human bronchial epithelial cells exposed to pulmonary surfactant. We conclude that prostaglandin E2 and its EP2 and EP4 receptors are likely involved in the relaxant effect of pulmonary surfactant in airways.