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  1. Abstract. Even though the Arctic is remote, aerosol properties observed there arestrongly influenced by anthropogenic emissions from outside the Arctic. Thisis particularly true for the so-called Arctic haze season (January throughApril). In summer (June through September), when atmospheric transportpatterns 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 emissionshave taken place. At the same time a large body of literature shows evidencethat the Arctic is undergoing fundamental environmental changes due toclimate forcing, leading to enhanced emissions by natural processes that mayimpact aerosol properties. In this study, we analyze 9 aerosol chemical species and 4 particleoptical properties from 10 Arctic observatories (Alert, Kevo, Pallas,Summit, Thule, Tiksi, Barrow/Utqiaġvik, Villum, and Gruvebadet and ZeppelinObservatory – both at Ny-Ålesund Research Station) to understand changesin anthropogenic and natural aerosol contributions. Variables includeequivalent black carbon, particulate sulfate, nitrate, ammonium,methanesulfonic acid, sodium, iron, calcium and potassium, as well asscattering and absorption coefficients, single scattering albedo andscattering Ångström exponent. First, annual cycles are investigated, which despite anthropogenic emissionreductions still show the Arctic haze phenomenon. Second, long-term trendsare studied using the Mann–Kendall Theil–Sen slope method. We find in total41 significant trends over full station records, i.e., spanning more than adecade, compared to 26 significant decadal trends. The majority ofsignificantly declining trends is from anthropogenic tracers and occurredduring the haze period, driven by emission changes between 1990 and 2000.For the summer period, no uniform picture of trends has emerged. Twenty-sixpercent of trends, i.e., 19 out of 73, are significant, and of those 5 arepositive and 14 are negative. Negative trends include not only anthropogenictracers such as equivalent black carbon at Kevo, but also natural indicatorssuch as methanesulfonic acid and non-sea-salt calcium at Alert. Positivetrends are observed for sulfate at Gruvebadet. No clear evidence of a significant change in the natural aerosolcontribution can be observed yet. However, testing the sensitivity of theMann–Kendall Theil–Sen method, we find that monotonic changes of around 5 % yr−1 in an aerosol property are needed to detect a significanttrend within one decade. This highlights that long-term efforts well beyonda decade are needed to capture smaller changes. It is particularly importantto understand the ongoing natural changes in the Arctic, where interannualvariability can be high, such as with forest fire emissions and theirinfluence on the aerosol population. To investigate the climate-change-induced influence on the aerosolpopulation and the resulting climate feedback, long-term observations oftracers more specific to natural sources are needed, as well as of particlemicrophysical properties such as size distributions, which can be used toidentify changes in particle populations which are not well captured bymass-oriented methods such as bulk chemical composition. 
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  2. null (Ed.)
    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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  3. null (Ed.)
    Abstract. Despite the potential importance of black carbon (BC) for radiative forcing of the Arctic atmosphere, vertically resolved measurements of the particle light scattering coefficient (σsp) and light absorption coefficient (σap) in the springtime Arctic atmosphere are infrequent, especially measurements at latitudes at or above 80∘ N. Here, relationships among vertically distributed aerosol optical properties (σap, σsp and single scattering albedo or SSA), particle microphysics and particle chemistry are examined for a region of the Canadian archipelago between 79.9 and 83.4∘ N from near the surface to 500 hPa. Airborne data collected during April 2015 are combined with ground-based observations from the observatory at Alert, Nunavut and simulations from the Goddard Earth Observing System (GEOS) model, GEOS-Chem, coupled with the TwO-Moment Aerosol Sectional (TOMAS) model (collectively GEOS-Chem–TOMAS; Kodros et al., 2018) to further our knowledge of the effects of BC on light absorption in the Arctic troposphere. The results are constrained for σsp less than 15 Mm−1, which represent 98 % of the observed σsp, because the single scattering albedo (SSA) has a tendency to be lower at lower σsp, resulting in a larger relative contribution to Arctic warming. At 18.4 m2 g−1, the average BC mass absorption coefficient (MAC) from the combined airborne and Alert observations is substantially higher than the two averaged modelled MAC values (13.6 and 9.1 m2 g−1) for two different internal mixing assumptions, the latter of which is based on previous observations. The higher observed MAC value may be explained by an underestimation of BC, the presence of small amounts of dust and/or possible differences in BC microphysics and morphologies between the observations and model. In comparing the observations and simulations, we present σap and SSA, as measured, and σap∕2 and the corresponding SSA to encompass the lower modelled MAC that is more consistent with accepted MAC values. Median values of the measured σap, rBC and the organic component of particles all increase by a factor of 1.8±0.1, going from near-surface to 750 hPa, and values higher than the surface persist to 600 hPa. Modelled BC, organics and σap agree with the near-surface measurements but do not reproduce the higher values observed between 900 and 600 hPa. The differences between modelled and observed optical properties follow the same trend as the differences between the modelled and observed concentrations of the carbonaceous components (black and organic). Model-observation discrepancies may be mostly due to the modelled ejection of biomass burning particles only into the boundary layer at the sources. For the assumption of the observed MAC value, the SSA range between 0.88 and 0.94, which is significantly lower than other recent estimates for the Arctic, in part reflecting the constraint of σsp<15 Mm−1. The large uncertainties in measuring optical properties and BC, and the large differences between measured and modelled values here and in the literature, argue for improved measurements of BC and light absorption by BC and more vertical profiles of aerosol chemistry, microphysics and other optical properties in the Arctic. 
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