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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.

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 mid-latitudes. 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 days, and CCN concentrations were measured over a period of 95 days. Continuous particle number size distributions were recorded, facilitating calculations of aerosol CCN activation diameters and aerosol kappa (κ)-values. In spring, average CCN concentrations, at supersaturations (SS) 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 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. This emphasizes the importance of accumulation mode aerosol sources to provide available CCN during summer. The influence of particle hygroscopic growth on the radiative transfer through aerosol-radiation interactions could be of major importance. The results of this study are directly applicable in the modeling of direct and indirect climate effects of Arctic aerosols. Targeted chemical and morphological analysis, based on filter samples or on-line techniques, could further clarify the role of primary organic marine influence on Arctic aerosol CCN concentrations and therewith climate effects.

To fight against the first wave of Coronavirus disease 2019 (COVID-19) in 2020, lockdown measures were implemented in most European countries. These lockdowns had well-documented effects on human mobility. We assessed the impact of the lockdown implementation and relaxation on air pollution by comparing daily particulate matter (PM), nitrogen dioxide (NO2), and ozone (O3) concentrations, as well as particle number size distributions (PNSD) and particle light absorption coefficients in-situ measurement data with values expected if no COVID-19 epidemic had occurred at 28 sites across Europe for the period 17 February – 31 May 2020. Expected PM, NO2 and O3 concentrations were calculated from the 2020 Copernicus Atmospheric Monitoring Service (CAMS) Ensemble forecasts, combined with 2019 CAMS Ensemble forecasts and measurement data. On average, lockdown implementations did not lead to a decrease in PM2.5 mass concentrations at urban sites, while relaxations resulted in a +26 ± 21% rebound. The impacts of lockdown implementation and relaxation on NO2 concentrations were more consistent (−29 ± 17 %, and +31 ± 30 %, respectively). The implementation of the lockdown measures also induced statistically significant increases in O3 concentrations at half of all sites (+13 % on average). An enhanced oxidizing capacity of the atmosphere could have boosted the production of secondary aerosol at those places. Changes in the wavelength dependence of the particle light absorption coefficients and PNSD were also examined at 14 and 13 sites, respectively. Since these variables are not calculated by the CAMS model, expected values were estimated from 2017–2019 measurement data. A significant change in the relative contributions of wood and fossil fuel burning to the concentration of black carbon during the lockdown was detected at 7 sites. The contribution of particles smaller than 70 nm to the total number of particles significantly changed at most of the urban sites, with a mean decrease of −7 ± 5 % coinciding with the lockdown implementation. Our study shows that the response of PM2.5 and PM10 mass concentrations to lockdown measures was not systematic at various sites across Europe for multiple reasons, the relationship between road traffic intensity and particulate air pollution being more complex than expected.

16 pages, 6 figures, 1 table, supplement https://doi.org/10.5194/acp-23-2183-2023-supplement.-- Code and data availability: The code and data used to produce all non-illustrative figures are available from the corresponding authors under reasonable request., 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, This research has been supported by the Ministerio de Economía y Competitividad (grant nos. CTM2017-89117-R, CGL2013-49020-R, and RYC-2012-11922), the Natural Environment Research Council (grant no. NE/S00579X/1), and the National Centre for Atmospheric Science funded by the Natural Environment Research Council. We acknowledge support of the publication fee by the CSIC Open Access Publication Support Initiative through its Unit of Information Resources for Research (URICI), With the institutional support of the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000928-S)

27 pages, 12 figures, supplement https://doi.org/10.5194/acp-23-389-2023.-- Data availability: All data sets used in this work that were obtained during the MOSAiC campaign will be made publicly available by 1 January 2023 via PANGAEA (https://www.pangaea.de/, last access: June 2022) or are already publicly available in the Department of Energy Atmospheric Radiation Measurement program (ARM) user facility data discovery tool (https://adc.arm.gov/discovery/#/, last access: March 2022). Data from the PANGAEA archive include the following. Meteorological observations from Polarstern: Schmithüsen, H.: Continuous meteorological surface measurement during POLARSTERN cruise PS122/1. Alfred Wegener Institute, Helmholtz Centre for Polar and Marine Research, Bremerhaven, PANGAEA [data set], https://doi.org/10.1594/PANGAEA.935221, 2021a. Schmithüsen, H.: Continuous meteorological surface measurement during POLARSTERN cruise PS122/2. Alfred Wegener Institute, Helmholtz Centre for Polar and Marine Research, Bremerhaven, PANGAEA [data set], https://doi.org/10.1594/PANGAEA.935222, 2021b. Schmithüsen, H.: Continuous meteorological surface measurement during POLARSTERN cruise PS122/3. Alfred Wegener Institute, Helmholtz Centre for Polar and Marine Research, Bremerhaven, PANGAEA [data set], https://doi.org/10.1594/PANGAEA.935223, 2021c. Schmithüsen, H.: Continuous meteorological surface measurement during POLARSTERN cruise PS122/4. Alfred Wegener Institute, Helmholtz Centre for Polar and Marine Research, Bremerhaven, PANGAEA [data set], https://doi.org/10.1594/PANGAEA.935224, 2021d. Schmithüsen, H.: Continuous meteorological surface measurement during POLARSTERN cruise PS122/5. Alfred Wegener Institute, Helmholtz Centre for Polar and Marine Research, Bremerhaven, PANGAEA [data set], https://doi.org/10.1594/PANGAEA.935225, 2021e. Black carbon (BC): Heutte, B., Beck, I., Quéléver, L., Jokinen, T., Laurila, T., Dada, L., Schmale, J.: Equivalent black carbon concentration in 10 minutes time resolution, measured in the Swiss container during MOSAiC 2019/2020, PANGAEA [data set], https://doi.org/10.1594/PANGAEA.952251, 2022. Particle number concentration (CPC3025): Beck, I., Quéléver, L., Laurila, T., Jokinen, T., and Schmale, J.: Continuous corrected particle number concentration data in 10 sec resolution, measured in the Swiss aerosol container during MOSAiC 2019/2020, PANGAEA [data set], https://doi.org/10.1594/PANGAEA.941886, 2022b. The ARM data include the following: Kuang, C., Singh, A., and Howie, J.: Scanning mobility particle sizer (AOSSMPS), ARM [data set], https://doi.org/10.5439/1476898, 2022. Kuang, C., Salwen, C., Boyer, M., and Singh, A.: Condensation Particle Counter (AOSCPCF), ARM [data set], https://doi.org/10.5439/1046184, 2022. The land-based PNSD data: Alert: Personal communication from Tak Chan and Sangeeta Sharma, 2022 (for details, see Croft et al., 2016). Villum: Personal communication from Jakob Boyd Pernov, 2022 (for details, see Nguyen et al., 2016). Zeppelin: Personal communication from Peter Tunved, 2022 (for details, see Tunved et al., 2013). Tiksi: Personal communication from Eija Asmi, 2022 (for details, see Asmi et al., 2016). Utqiaġvik: Freud, E., Krejci, R., Tunved, P., Leaitch, W. R., Nguyen, Q. T., Massling, A., Skov, H., and Barrie, L.: Hourly mean homogenised (dry diameter range 20 to 500 nm) observations of aerosol number size distributions from station Barrow, 2007-09-20 to 2015-07-09, PANGAEA [data set], https://doi.org/10.1594/PANGAEA.877329, 2017b. The land-based BC data: Villum: Personal communications from Daniel Thomas, Jakob Klenø Nøjgaard, and Andreas Massling, 2022 (for details, see Thomas et al., 2022). NOAA Barrow Atmospheric Baseline Observatory (Utqiaġvik) during 2020: personal communication from Elisabeth Andrews, 2022 (for processing details, see Schmale et al., 2022). Gruvebadet. The PSAP data are accessible at the Italian Arctic Data Center operated by the National Research Council of Italy: https://data.iadc.cnr.it/erddap/tabledap/ebc_2010_2020.html (last access: December 2021, refer to Schmale et al., 2022, for additional details). All other BC data sets used in this work will be made publicly available on EBAS (http://ebas-data.nilu.no/, last access: December 2021, refer to Schmale et al., 2022, for additional details). The Arctic Oscillation (AO) data are publicly available from the NOAA and the National Weather Service: https://www.cpc.ncep.noaa.gov/products/precip/CWlink/daily_ao_index/ao.shtml (last access: June 2022). An archive of the FLEXPART model output and quick looks for the whole campaign can be found at https://img.univie.ac.at/webdata/mosaic (last access: March 2022), The Arctic environment is rapidly changing due to accelerated warming in the region. The warming trend is driving a decline in sea ice extent, which thereby enhances feedback loops in the surface energy budget in the Arctic. Arctic aerosols play an important role in the radiative balance and hence the climate response in the region, yet direct observations of aerosols over the Arctic Ocean are limited. In this study, we investigate the annual cycle in the aerosol particle number size distribution (PNSD), particle number concentration (PNC), and black carbon (BC) mass concentration in the central Arctic during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition. This is the first continuous, year-long data set of aerosol PNSD ever collected over the sea ice in the central Arctic Ocean. We use a k-means cluster analysis, FLEXPART simulations, and inverse modeling to evaluate seasonal patterns and the influence of different source regions on the Arctic aerosol population. Furthermore, we compare the aerosol observations to land-based sites across the Arctic, using both long-term measurements and observations during the year of the MOSAiC expedition (2019–2020), to investigate interannual variability and to give context to the aerosol characteristics from within the central Arctic. Our analysis identifies that, overall, the central Arctic exhibits typical seasonal patterns of aerosols, including anthropogenic influence from Arctic haze in winter and secondary aerosol processes in summer. The seasonal pattern corresponds to the global radiation, surface air temperature, and timing of sea ice melting/freezing, which drive changes in transport patterns and secondary aerosol processes. In winter, the Norilsk region in Russia/Siberia was the dominant source of Arctic haze signals in the PNSD and BC observations, which contributed to higher accumulation-mode PNC and BC mass concentrations in the central Arctic than at land-based observatories. We also show that the wintertime Arctic Oscillation (AO) phenomenon, which was reported to achieve a record-breaking positive phase during January–March 2020, explains the unusual timing and magnitude of Arctic haze across the Arctic region compared to longer-term observations. In summer, the aerosol PNCs of the nucleation and Aitken modes are enhanced; however, concentrations were notably lower in the central Arctic over the ice pack than at land-based sites further south. The analysis presented herein provides a current snapshot of Arctic aerosol processes in an environment that is characterized by rapid changes, which will be crucial for improving climate model predictions, understanding link, This research has been supported by the Academy of Finland (grant no. 337552), Horizon 2020 (EMME-CARE, grant no. 856612), the US Department of Energy (grant no. DE-SC0022046), and the Swiss Polar Institute (grant no. 188478), With the institutional support of the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000928-S)

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-yearlong 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., Atmospheric Chemistry and Physics, 23 (8), ISSN:1680-7375, ISSN:1680-7367

Air pollution is associated with increased risk of myocardial infarction (MI), but it is unresolved to what extent the association is modified by factors such as socioeconomic status, comorbidities, financial stress, residential green space, or road traffic noise. We formed a cohort of all (n = 1,964,702) Danes, aged 50–85 years, with 65,311 cases of MI during the followed-up period 2005–2017. For all participants we established residential five-year running average exposure to particulate matter 2.5), ultrafine particles (UFP, 2). We evaluated risk in population strata, using Aalen additive hazards models to estimate absolute risk and Cox proportional hazards models to estimate relative risk of MI with 95% confidence intervals (CI). PM2.5 and the other pollutant were associated with MI. Lower education and lower income were associated with higher absolute risks of MI from air pollution, whereas no clear effect modification was apparent for relative risk estimates. For example, 5 μg/m3 higher PM2.5 was associated with HR for MI of 1.16 (95% CI: 1.10–1.22) among those with only mandatory education and 1.13 (95% CI: 1.03–1.24) among those with long education. The corresponding rate differences per 100,000 person years were 243 (95% CI: 216–271) and 358 (95% CI: 338–379), respectively. Higher level of comorbidity was consistently across all four pollutants associated with both higher absolute and relative risk of MI. In conclusion, people with comorbid conditions or of lower SES appeared more vulnerable to long-term exposure to air pollution and more cases of MI may be prevented by focused interventions in these groups.

The Arctic environment is rapidly changing due to accelerated warming in the region. The warming trend is driving a decline in sea ice extent, which thereby enhances feedback loops in the surface energy budget in the Arctic. Arctic aerosols play an important role in the radiative balance, and hence the climate response, in the region; yet direct observations of aerosols over the Arctic Ocean are limited. In this study, we investigate the annual cycle in the aerosol particle number size distribution (PNSD), particle number concentration (PNC), and black carbon (BC) mass concentration in the central Arctic during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition. This is the first continuous, year-long dataset of aerosol PNSD ever collected over the sea ice in the central Arctic Ocean. We use a k-means cluster analysis, FLEXPART simulations, and inverse modeling to evaluate seasonal patterns and the influence of different source regions on the Arctic aerosol population. Furthermore, we compare the aerosol observations to land-based sites across the Arctic, using both long-term measurements and observations during the year of the MOSAiC expedition (2019–2020), to investigate interannual variability and to give context to the aerosol characteristics from within the central Arctic. Our analysis identifies that, overall, the central Arctic exhibits typical seasonal patterns of aerosols, including anthropogenic influence from Arctic Haze in winter and secondary aerosol processes in summer. The seasonal pattern corresponds with the global radiation, surface air temperature, and the timing of sea ice melting/freezing, which drives changes in transport patterns and secondary aerosol processes. In winter, the Norilsk region in Russia/Siberia was the dominant source of Arctic Haze signal in the PNSD and BC observations, which contributed to higher accumulation mode PNC and BC mass concentration in the central Arctic than at land-based observatories. We also show that the wintertime Arctic Oscillation (AO) phenomenon, which was reported to achieve a record-breaking positive phase during January–March 2020, explains the unusual timing and magnitude of Arctic Haze across the Arctic region compared to longer-term observations. In summer, the PNC of nucleation and Aitken mode aerosol is enhanced, but concentrations were notably lower in the central Arctic over the ice pack than at land-based sites further south. The analysis presented herein provides a current snapshot of Arctic aerosol processes in an environment that is characterized by rapid changes, which will be crucial for improving climate model predictions, understanding linkages between different environmental processes, and investigating the impacts of climate change in future Arctic aerosol studies.

International audience; Integrative and Comprehensive Understanding on Polar Environments (iCUPE) project developed 24 novel datasets utilizing in-situ observational capacities within the Arctic or remote sensing observations from ground or from space. The datasets covered atmospheric, cryospheric, marine, and terrestrial domains. This paper connects the iCUPE datasets to United Nations’ Sustainable Development Goals and showcases the use of selected datasets as knowledge provision services for policy- and decision-making actions. Inclusion of indigenous and societal knowledge into the data processing pipelines enables a feedback mechanism that facilitates data driven public services.

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 provide a climate forcing effect. NPF has been studied comprehensively at different sites in the Arctic ranging from those in the high Arctic, those at Svalbard, and those in the continental Arctic, but no harmonized 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, Mt. Zeppelin, Gruvebadet. & Utqiagvik). Our analysis of particle formation and growth rates, as well as back trajectory analysis shows summertime maxima in frequency of NPF and particle formation rate at all sites, although the mean frequency and particle formation rates themselves vary greatly between sites, highest at Svalbard, and lowest in the high Arctic. 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 masse 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 emphasize how understanding the geographical variation in surface type across the Arctic is key to understanding secondary aerosol sources, and provide a harmonised analysis of NPF across the Arctic.

Dimethyl sulfide (DMS) is emitted by phytoplankton species in the oceans and constitutes the largest source of naturally emitted sulfur to the atmosphere. The climate impact of secondary particles, formed through the oxidation of DMS by hydroxyl radicals, is still elusive. This study investigates the hygroscopicity and cloud condensation nuclei activity of such particles and discusses the results in relation to their chemical composition. We show that mean hygroscopicity parameters, κ, during an experiment for particles of 80 nm in diameter range from 0.46 to 0.52 or higher, as measured at both sub- and supersaturated water vapour conditions. Ageing of the particles leads to an increase in κ from, for example, 0.50 to 0.58 over the course of 3 h (Exp. 7). Aerosol mass spectrometer measurements from this study indicate that this change most probably stems from a change in chemical composition leading to slightly higher fractions of ammonium sulfate compared to methanesulfonic acid (MSA) within the particles with ageing time. Lowering the temperature to 258 K increases κ slightly, particularly for small particles. These κ values are well comparable to previously reported model values for MSA or mixtures between MSA and ammonium sulfate. Particle nucleation and growth rates suggest a clear temperature dependence, with slower rates at cold temperatures. Quantum chemical calculations show that gas-phase MSA clusters are predominantly not hydrated, even at high humidity conditions, indicating that their gas-phase chemistry should be independent of relative humidity.

IntroductionThe Arctic region is particularly sensitive to global climate change, experiencing warming at twice the rate of the global average. Changes within and outside of the Arctic (e.g., meteorology, atmospheric transport, and precipitation patterns) can have consequences for the sources and sinks of aerosols. Atmospheric aerosols can alter the planetary radiation balance directly through scattering and absorption and indirectly through modification of cloud properties. Understanding the direction and magnitude of recent changes in the Arctic aerosol population is key to elucidating the implications for the changing Arctic, although this remains a scientific challenge. Here we report a Pan-Arctic view of recent trends for aerosol particle number concentrations in different size fractions. Measurement Site & MethodsMeasurements were obtained from different stations around the Arctic including Villum Research Station (Villum, 81°36’ N, 16°39’ W, 24 m a.s.l) in northeastern Greenland, Alert (81°28’ N, 62°30’ W, 210 m a.s.l.) in the Canadian Archipelago, Zeppelin Observatory (78°56’ N, 11°53’ E, 474 m a.s.l.) on Svalbard, Pallas (67°58’N, 24°07’ E, 560 m a.s.l.) in northern Finland, and Tiksi (71°36’ N, 128°53’E, 1 m a.s.l.) in the Siberian Arctic.Particle number size distributions (PNSD) were measured using a Scanning Mobility Particle Sizer (SMPS) at Villum and Alert, and a Differential Mobility Particle Sizer (DMPS) at Zeppelin, Pallas, and Tiksi. Measurements were collected from 2010 to 2018 at all sites except for Zeppelin (2011 to 2019). Number concentrations were calculated by integrating the PNSD for three size fractions: Nucleation (10-35 nm), Aitken (35-80 nm), and Accumulation (80-300 nm). Nucleation number concentrations were unavailable for Zeppelin.The trends in the number concentration for these size fractions were identified and quantified using the Mann-Kendal test and Theil Sen slope on the 90th % confidence interval via the 3PW algorithm, using the daily median as temporal aggregation and meteorological seasons as temporal segmentation. Only statistically significant trends are discussed. ResultsAlthough the sites Villum, Alert, and Zeppelin are all located in the High Arctic (> 75° N) and relatively close to one another, there are differences between the direction and magnitude of trends for the size fractions. For example, at Villum, increasing trends are observed for the Nucleation fraction during spring and summer. Interestingly, at Alert, decreasing trends are observed for the Accumulation fraction during spring and autumn. At Zeppelin, no significant trends were observed for any fraction during any season. Similar to the High Arctic sites, for the continental sites, Tiksi and Pallas, no uniform picture for the direction and magnitude of trends in the size fractions is observed. At Tiksi, decreasing trends for both the Aitken and Accumulation fractions are detected during summer and autumn. While at Pallas, no significant trends were observed during any season. This work offers insight into the climatic implications (i.e., radiative balance and cloud properties) for a future Arctic climate by monitoring changes of aerosol concentrations in optically and cloud-relevant sizes. Future work will investigate the causes of these trends.

Despite a large number of studies, 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 different sizes in total of for 21 measurement sites in Europe and Arctic. For 13 of those, 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 (ESM). 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, were typically stronger in 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, for others, 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 showing clear differences in concentrations between remote and urban sites. To conclude, although anthropogenic mass emissions are harmonized in models, trends in different sized particles vary among the model 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.

Magnesium and calcium chloride salts contribute to the global atmospheric aerosol burden via emission of sea spray and mineral dust. Their influence on aerosol hygroscopicity and cloud forming potential is important but uncertain with ambiguities between results reported in the literature. To address this, we have conducted measurements of the hygroscopic growth and critical supersaturation of dried, size selected nano-particles made from aqueous solution droplets of MgCl2 and CaCl2, respectively, and compare experimentally derived values with results from state-of-the-art thermodynamic modelling. It is characteristic of both MgCl2 and CaCl2 salts that they bind water in the form of hydrates under a range of ambient conditions. We discuss how hydrate formation affects the particles' water uptake and provide an expression for hydrate correction factors needed in calculations of hygroscopic growth factors, critical super-saturations, and derived κ values of particles containing hydrate forming salts. We demonstrate the importance of accounting for hydrate forming salts when predicting hygroscopic properties of sea spray aerosol.

The Arctic atmosphere is warming rapidly and its relatively pristine environment is sensitive to the long-range transport of atmospheric pollutants. While carbon dioxide is the main cause for global warming, short-lived climate forcers (SLCFs) such as methane, ozone, and particles also play a role in Arctic climate on near-term time scales. Atmospheric modelling is critical for understanding the abundance and distribution of SLCFs throughout the Arctic atmosphere, and is used as a tool towards determining 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, 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 four years (2008–2009 and 2014–2015) conducted for the 2021 Arctic Monitoring and Assessment Programme (AMAP) SLCF assessment report are thoroughly evaluated against satellite, ground, ship and aircraft-based observations. 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 was able to represent the general features of SLCFs in the Arctic, though vertical mixing, long-range transport, deposition, and wildfire emissions remain highly uncertain processes. These need better representation within atmospheric models to improve their simulation of SLCFs in the Arctic environment.

Organic aerosols in the Arctic are predominantly fuelled by anthropogenic sources in winter and natural sources in summer, according to observations from eight sites across the Arctic Aerosols play an important yet uncertain role in modulating the radiation balance of the sensitive Arctic atmosphere. Organic aerosol is one of the most abundant, yet least understood, fractions of the Arctic aerosol mass. Here we use data from eight observatories that represent the entire Arctic to reveal the annual cycles in anthropogenic and biogenic sources of organic aerosol. We show that during winter, the organic aerosol in the Arctic is dominated by anthropogenic emissions, mainly from Eurasia, which consist of both direct combustion emissions and long-range transported, aged pollution. In summer, the decreasing anthropogenic pollution is replaced by natural emissions. These include marine secondary, biogenic secondary and primary biological emissions, which have the potential to be important to Arctic climate by modifying the cloud condensation nuclei properties and acting as ice-nucleating particles. Their source strength or atmospheric processing is sensitive to nutrient availability, solar radiation, temperature and snow cover. Our results provide a comprehensive understanding of the current pan-Arctic organic aerosol, which can be used to support modelling efforts that aim to quantify the climate impacts of emissions in this sensitive region.

The outbreak of SARS-CoV-2 and subsequent spread of the disease COVID-19 became classified as a pandemic in March of 2020, leading to global safety measures introduced to limit the impact of the virus. This combination of safety measures has become commonly referred to as “lockdown”. The associated industry and lifestyle changes led to reductions in the anthropogenic emission of atmospheric pollutants such as black carbon (BC), which is transported from the mid-latitudes into the Arctic during the winter and spring. Measurements of BC and other anthropogenic pollutants are of increasing importance in the Arctic due to the rapid warming observed there in the past few decades. It is believed that BC has a significant role in this warming, and so understanding the Arctic's response to reduced BC emissions at lower latitudes will provide insight into how future changes might mitigate further warming. Reductions in BC have been reported worldwide, and so in this study, the impact of these reductions on BC concentrations at the High Arctic site Villum Research Station was investigated. The effect was examined from March 2020, around when global lockdowns began, to June 2020, when the Arctic haze period ended and BC levels were once again low. Firstly, the Danish Eulerian Hemispheric Model (DEHM) was used to assess this impact on BC concentrations by adjusting global anthropogenic pollution emission inventories to simulate those observed during the lockdown period and comparing the results to a similar model run with standard emission inventories. Secondly, equivalent BC data from an aethalometer at Villum Research Station were analysed, comparing the concentrations during the lockdown period to both aethalometer data from previous years and DEHM results from the lockdown period. It was found that when adjusted DEHM emission inventories were introduced from the 1st of March, the model predicted a reduction in BC concentrations beginning on the 10th of March and reached a 10% reduction by the 1st of April. This reduction fluctuated around 10% until the end of the Arctic haze period. Aethalometer data did not show any significant change from previous years, and no concentration reduction could be concluded from its comparison with DEHM results. This is likely because the predicted reduction of 10% is smaller than both the inter-annual and intra-annual variability of measured BC concentrations at Villum.

19 pages, 9 figures, 1 table, 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-rangetransported-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 northeastern 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 pro cesses 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, This research has been supported by the Spanish Ministry of Economy through project BIO-NUC (CGL2013-49020-R), PI-ICE (CTM2017-89117-R) and the Ramon y Cajal fellowship (RYC-2012-11922). The research leading to these results has received funding from the European Union's Horizon 2020 research and innovation programme under grant agreement no. 654109, the Danish Council for Independent Research (project NUMEN, DFF-FTP-4005-00485B) and previously from the European Union Seventh Framework Programme (FP7/2007-2013) under grant agreement no. 262254. The work at Villum Research Station, Station Nord, was financially supported by the Danish Environmental Protection Agency via the MIKA/DANCEA funds for Environmental Support to the Arctic Region. The Villum Foundation funded the construction of Villum Research Station, Station Nord. CCN measurements are supported by a KOPRI program (PN19081), funded by a National Research Foundation of Korea grant (NRF-2016M1A5A1901769). The authors acknowledge financial support (to David C. S. Beddows) from the Natural Environment Research Council's funding of the National Centre for Atmospheric Science (NCAS) (grant number R8/H12/83/011)

11 pages, supporting information https://doi.org/10.1021/acs.est.9b00991, The radiative balance in the Arctic region is sensitive to in-cloud processes, which principally depend on atmospheric aerosols, including ice nucleating particles (INPs). High temperature INPs (active at ≥−15 °C) are common in the Arctic. While laboratory and limited in situ studies show that the high-temperature active INPs are associated with bioaerosols and biogenic compounds, there is still little quantitative insight into the Arctic biogenic INPs and bioaerosols. We measured concentrations of bioaerosols, bacteria, and biogenic INPs at the Villum Research Station (VRS, Station Nord) in a large number of snow (15) and air (51) samples. We found that INPs active at high subzero temperatures were present both in spring and summer. Air INP concentrations were higher in summer (18 INP m–3 at ≥−10 °C) than in spring (

IntroductionThe Arctic region is particularly sensitive to global climate change, experiencing warming at twice the rate of the global average. Anthropogenic pollution (e.g. aerosols, black carbon, ozone, and greenhouse gases), which to a large extent originates from the mid-latitudes, is suspected to be partly responsible for this warming. Atmospheric aerosols can alter the planetary radiation balance directly through scattering and absorption and indirectly through modification of cloud properties. These interactions depend on aerosol physicochemical properties. The Arctic cryosphere and atmosphere has undergone significant changes in recent decades, accompanied by reductions in anthropogenic emissions, especially in Europe and North America. These changes have important ramifications for the ambient Arctic aerosol. Understanding the direction and magnitude of recent changes in the Arctic aerosol population is key to elucidating the implications for the changing Arctic, although this remains a scientific challenge. Here we report recent trends for aerosol particle physical properties, which will aid in this understanding of the changing Arctic.Measurement Site & MethodsAll measurements were obtained at Villum Research Station (Villum, N 81o36’ W 16o39’ 24 m a.s.l) in northeastern Greenland. Particle number size distributions (PNSD) were measured using a Scanning Mobility Particle Sizer (SMPS) from 2010–2018.We have utilized mode fitting on daily averaged PNSDs to characterize three distinct modes (Nucleation, Aitken, and Accumulation) along with geometric mean diameters (GMD) and number concentrations (PN) for each mode.The trends in these parameters were identified and quantified using the Mann-Kendal test and Theil Sen slope on the 90th % confidence interval. Trends in different months were analyzed using daily modal parameters.ResultsStatistically significant (s.s.) decreasing trends were detected for the Nucleation and Aitken modes GMDs in the winter, spring, and summer, with the only s.s. increasing trends occurring in the autumn. The Accumulation mode GMD showed a s.s. decrease in the spring and s.s. increase in the summer. For the PN of each mode, large s.s. increasing trends were detected for Nucleation and Aitken mode PN in the spring and summer. The Accumulation mode PN showed a small s.s. increase in the summer and a large s.s. decrease in the autumn. These results show that ultrafine modes (Nucleation and Aitken) are decreasing in diameter while simultaneously increasing in number concentration. These trends are most likely related to changes in sea ice extent, as previous research has indicated a negative correlation between new particle formation and sea ice extent. The decrease in Accumulation mode GMD in spring (during the peak of the Arctic Haze) is possibly related to decreases in anthropogenic emissions, while the increase PN during summer could signal an increase in primary biogenic aerosol emissions from the ocean surface. The large decrease in Accumulation mode PN during autumn requires further investigation. This work will help confirm trends of other aerosol components observed at other High Arctic sites and can offer insight into the climatic implications (i.e., radiative balance and cloud properties) for a future Arctic climate.

11 pags., 4 figs., New particle formation in the Arctic atmosphere is an important source of aerosol particles. Understanding the processes of Arctic secondary aerosol formation is crucial due to their significant impact on cloud properties and therefore Arctic amplification. We observed the molecular formation of new particles from low-volatility vapors at two Arctic sites with differing surroundings. In Svalbard, sulfuric acid (SA) and methane sulfonic acid (MSA) contribute to the formation of secondary aerosol and to some extent to cloud condensation nuclei (CCN). This occurs via ion-induced nucleation of SA and NH and subsequent growth by mainly SA and MSA condensation during springtime and highly oxygenated organic molecules during summertime. By contrast, in an ice-covered region around Villum, we observed new particle formation driven by iodic acid but its concentration was insufficient to grow nucleated particles to CCN sizes. Our results provide new insight about sources and precursors of Arctic secondary aerosol particles., The authors acknowledge European Research Council (GASPARCON, Grant no. 714621 and COALA, Grant no. 638703), Academy of Finland (Project nos. 296628, 306853, 317380, 316114, and 320094), INTERACT, European Regional Development Fund (project MOBTT42), Austrian Science Fund (FWF, Project J3951-N36), the European Union's Horizon 2020 Research and Innovation Program (Grant no. 689443) via project iCUPE (Integrative and Comprehensive Understanding on Polar Environments) and Project ERC-2016- COG 726349 CLIMAHAL, National Research Foundation (NRF) of the Ministry of Science, ICT and Future Planning (NRF-2018R1A2A1A19019281), Knut-and-Alice-Wallenberg Foundation within the Arctic Climate Across Scales (Project No. \,2016.0024), the Swedish EPA's (Naturvårdsverket) Environmental monitoring program (Miljöövervakning), the Swedish Research Council FORMAS (Project "Interplay between water, clouds and Aerosols in the Arctic," \# 2016-01427), Climate Change Tower – Integrated Project of the National Research Council of Italy and the National Interest Project by the Italian Minister of Education, University and Research (PRIN2007 and PRIN2009). The authors thank Department of Earth System Sciences and Technologies for the Environment, Department of Earth Sciences and Technology of the Environment of CNR and the doctoral program in atmospheric sciences at the University of Helsinki for financial support. Aarhus University acknowledge financial support from Danish Ministry of Environment and food and Ministry of Climate, Energy and Utilities by means of DANCEA.

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, i.e. natural sources of aerosols and precursors, play an important role. Over the last 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 nine aerosol chemical species and four particle optical properties from ten Arctic observatories (Alert, Gruvebadet, Kevo, Pallas, Summit, Thule, Tiksi, Barrow, Villum, Zeppelin) 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 28 significant trends over full station records, i.e. spanning more than a decade, compared to 17 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-one percent of trends, i.e. eleven out of 57, are significant, and of those five are positive and six 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 Zeppelin and 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 % per year 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.

Sea spray aerosol (SSA) contributes significantly to natural aerosol particle concentrations globally, in marine areas even dominantly. The potential changes of the omnipresent inorganic fraction of SSA due to atmospheric ageing is largely unexplored. We demonstrate that ageing of liquid NaCl and artificial sea salt aerosol by exposure to ozone and UV light leads to a substantial decrease in hygroscopicity and cloud activation potential. The results point towards surface reactions that are more crucial for small particles and the formation of salt structures with water bound within the aerosols, termed hydrates. Our findings suggest an increased formation of hydrate forming salts during ageing and the presence of hydrates in dried SSA. Field observations indicate a reduced hygroscopic growth of sub-micrometre SSA in the marine atmosphere compared to pure NaCl which is typically attributed to organic matter or sulphates. Aged inorganic sea salt offers an additional explanation for reduced hygroscopicity and cloud activation potential.

New particle formation (NPF) events occur almost everywhere in the world and can play an important role as a particle source. The frequency and characteristics of NPF events vary spatially and this variability is yet to be fully understood. In the present study, long term particle size distribution datasets (minimum of three years) from thirteen sites of various land uses and climates from across Europe were studied and NPF events, deriving from secondary formation and not traffic related nucleation, were extracted and analysed. The frequency of NPF events was consistently found to be higher at rural background sites, while the growth and formation rates of newly formed particles were higher at roadsides, underlining the importance of the abundance of condensable compounds of anthropogenic origin found there. The growth rate was higher in summer at all rural background sites studied. The urban background sites presented the highest uncertainty due to greater variability compared to the other two types of site. The origin of incoming air masses and the specific conditions associated with them greatly affect the characteristics of NPF events. In general, cleaner air masses present higher probability for NPF events, while the more polluted ones show higher growth rates. However, different patterns of NPF events were found even at sites in close proximity (

Although new particle formation (NPF) events have been studied extensively for some decades, the mechanisms that drive their occurrence and development are yet to be fully elucidated. Laboratory studies have done much to elucidate the molecular processes involved in nucleation, but this knowledge has yet to be linked to NPF events in the atmosphere, except at very clean air sites. There is great difficulty in successful application of the results from laboratory studies to real atmospheric conditions, due to the diversity of atmospheric conditions and observations found, as NPF events occur almost everywhere in the world without following a clearly defined trend of frequency, seasonality, atmospheric conditions or event development. The present study seeks common features in nucleation events by applying a binned linear regression over an extensive dataset from 16 sites of various types (rural and urban backgrounds as well as roadsides) in Europe. A clear positive relation is found between the solar radiation intensity, temperature and atmospheric pressure with the frequency of NPF events, while relative humidity presents a negative relation with NPF event frequency. Wind speed presents a less consistent relationship which appears to be heavily affected by local conditions. While some meteorological variables appear to have a crucial effect on the occurrence and characteristics of NPF events, especially at rural sites, it appears that their role becomes less marked when at higher values. The analysis of chemical composition data presents interesting results. Concentrations of almost all chemical compounds studied (apart from O3) and the Condensation Sink (CS) have a negative relation with NPF event probability, though areas with higher average concentrations of SO2 had higher NPF event probability. Particulate Organic Carbon (OC), Volatile Organic Compounds (VOCs) and particulate phase sulphate consistently had a positive relation with the growth rate of the newly formed particles. As with some meteorological variables, it appears that at increased concentrations of pollutants or the CS, their influence upon NPF probability is reduced.

The role of polar regions increases in terms of megatrends such as globalization, new transport routes, demography and use of natural resources consequent effects of 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 (EO) and multi-scale modeling to synthesize data from comprehensive long-term measurements, intensive campaigns and satellites to deliver data products, metrics and indicators to the 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 provision of novel data in atmospheric pollution, local sources and transboundary transport, characterization of arctic surfaces and their changes, assessment of concentrations and impacts of heavy metals and persistent organic pollutants and their cycling, quantification of emissions from natural resource extraction and 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 integration of comprehensive in situ observations, satellite remote sensing and multiscale modeling in the Arctic context.

Modelling of ambient particle number concentrations (PNC) has been implemented in the Danish air quality modelling system DEHM/UBM/AirGIS and evaluated with long-term measurements. We implemented particle dynamical processes in the regional scale model DEHM using the M7 aerosol dynamics module (presented in the accompanying article by Frohn et al., 2021), and we developed models for PNC at the local scale (UBM) and street scale (OSPM), in a first approximation without including the particle dynamics as presented in this article. Outdoor concentration estimates are provided at the front door of all residential address locations in Denmark for the past 40 years (1979–2018) with a spatial resolution of 1 km × 1 km taking all emission sectors in Denmark into account and additionally at the street location, with significant traffic (>500 vehicles/day). We evaluated our model with up to 18-year long measurement time series of particle number size distributions (PNSD) at Danish street, urban and rural background stations. Two particle size ranges were used for evaluation: PNC>10 (count of particles with diameter larger than 10 nm) and PNC30_250 (diameter range 30–250 nm), in order to exclude nucleation events from the measurements and to obtain a consistent long-term measured time series. When comparing our model estimates with PNC30_250 measurements, we obtain Pearson correlation coefficients (Rp) in the range 0.39–0.95 depending on station location (street, urban background, rural) and averaging time (hour, day, month, year). The highest correlations were found for yearly averages at a monitoring station located at a street with dense traffic (Rp = 0.95) whereas shorter time averages and comparisons with monitoring stations at urban and rural background locations provided lower correlations. The model performance for PNC in terms of correlation coefficients with respect to measurements is comparable to the performance for other pollutants such as NOX, PM2.5 and better than the performance for PM10. The model generally overestimated the observed concentrations, Normalized Mean Bias (NMB) was in the range 6%–190% compared to PNC>10 and 90%–290% compared to PNC30_250. These relatively high NMBs are probably caused by uncertainties in the modelling process, especially the estimation of particle number emissions, which largely determine the ambient concentrations of PNC. Furthermore, uncertainties might as well originate from the complexity of modelling particle dynamical processes accurately and the great challenges in performing long-term PNC measurements. The presented model can estimate PNC at all Danish addresses over the last 40 years with a 1-h time resolution. The data seem to provide a good indication of the relative differences in PNC at Danish addresses.

There are limited measurements of the chemical composition, abundance, and sources of black carbon (BC) containing particles in the high Arctic. To address this, we report 93 days of Soot Particle Aerosol Mass Spectrometer (SP-AMS) data collected in the high Arctic. The period spans from February 20th until May 23rd 2015 at Villum Research Station (VRS) in Northern Greenland (81°36' N). Particulate sulfate (SO42−) accounted for 66 % of the non-refractory PM1, which amounted to 2.3 µg m−3 as an average value observed during the campaign. The second most abundant species was organic matter (24 %), averaging 0.55 µg m3. Both organic aerosol (OA) and PM1, estimated from the sum of all collected species, showed a marked decrease throughout May in accordance with Arctic haze leveling off. The refractory black carbon (rBC) concentration averaged 0.1 µg m−3 over the entire campaign. 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, which accounted for 64 % of the OA and dominated until mid-April while being nearly absent from the end of May; and (3) a more oxygenated Marine Organic Aerosol (MOA) factor, which accounted for 22 % of OA. AOA correlated significantly with SO42−, suggesting the main part of that factor being 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. Important differences are observed among the factors, including the highest O/C ratio (0.95) and S/C ratio (0.011) for MOA – the marine related factor. Our data supports current understanding of the Arctic summer aerosols, driven mainly by secondary aerosol formation, but with an important contribution from marine emissions. In view of a changing Arctic climate with changing sea-ice extent, biogenic processes, and corresponding source strengths, highly time-resolved data are urgently needed in order to elucidate the components dominating aerosol concentrations.