The Arctic environment has changed profoundly in recent decades. Aerosol particles are involved in numerous feedback mechanisms in the Arctic, e.g., aerosol-cloud/radiation interactions, which have important climatic implications. To understand changes in different Arctic aerosol types and number concentrations, we have performed a trend analysis of particle number size distributions, their properties, and their associated air mass history at Villum Research Station, northeastern Greenland, from 2010 to 2018. We found that, during spring, the total/ultrafine mode number concentration and the time air masses spent over the open ocean is significantly increasing, which can be ascribed to transport patterns changing to more frequent arrival from the ice-free Greenland Sea. We found that, during summer, the total/ultrafine mode number concentration, the occurrence of the Nucleation cluster (i.e. newly formed particles from gas to particle conversion), and the time air masses spent over the open ocean is significantly increasing. This can also be attributed to changing transport patterns, here with air masses arriving more frequently from Baffin Bay. Finally, we found that, during autumn, the ultrafine number concentration and the occurrence of the Pristine cluster (i.e. clean, natural Arctic background conditions) is significantly increasing, which is likely due to increasing amounts of accumulated precipitation along the trajectory path and decreasing time air masses spent above the mixed layer, respectively. Our results demonstrate that changing circulation and precipitation patterns are the factors predominantly affecting the trends in aerosol particle number concentrations and the occurrence of different aerosol types in northeastern Greenland.

Abstract. 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 linkages between different environmental processes, and investigating the impacts of climate change in future Arctic aerosol studies.

Abstract. 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.

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Abstract. 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 introduced 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 ecosystem. Therefore, to further our understanding of the dynamics of gaseous oxidized mercury in the High Arctic during the late summer, we performed measurements of GEM and GOM along with meteorological parameters, atmospheric constituents, and air mass history during two summer campaigns in 2019 and 2020 at Villum Research Station (Villum) in Northeastern Greenland. Five events of enhanced GOM concentrations were identified and investigated in greater detail. The origin of these events was identified, through analysis of air mass back-trajectories, associated meteorological data, and other atmospheric constituents, to be the cold, dry free troposphere. These events were associated with low RH, limited precipitation, cold temperatures, and intense sunlight along the trajectory path. Events were positively correlated with ozone, aerosol particle number, and black carbon mass concentration, which were interpreted as an indication of tropospheric air masses. This work aims to provide a better understanding of the dynamics of GOM during the High Arctic summer.