Abstract. Motivated by the need to predict how the Arctic atmosphere will change in a warming world, this article summarizes recent advances made by the research consortium NETCARE (Network on Climate and Aerosols: Addressing Key Uncertainties in Remote Canadian Environments) that contribute to our fundamental understanding of Arctic aerosol particles as they relate to climate forcing. The overall goal of NETCARE research has been to use an interdisciplinary approach encompassing extensive field observations and a range of chemical transport, earth system, and biogeochemical models. Several major findings and advances have emerged from NETCARE since its formation in 2013. (1) Unexpectedly high summertime dimethyl sulfide (DMS) levels were identified in ocean water (up to 75 nM) and the overlying atmosphere (up to 1 ppbv) in the Canadian Arctic Archipelago (CAA). Furthermore, melt ponds, which are widely prevalent, were identified as an important DMS source (with DMS concentrations of up to 6 nM and a potential contribution to atmospheric DMS of 20 % in the study area). (2) Evidence of widespread particle nucleation and growth in the marine boundary layer was found in the CAA in the summertime, with these events observed on 41 % of days in a 2016 cruise. As well, at Alert, Nunavut, particles that are newly formed and grown under conditions of minimal anthropogenic influence during the months of July and August are estimated to contribute 20 % to 80 % of the 30–50 nm particle number density. DMS-oxidation-driven nucleation is facilitated by the presence of atmospheric ammonia arising from seabird-colony emissions, and potentially also from coastal regions, tundra, and biomass burning. Via accumulation of secondary organic aerosol (SOA), a significant fraction of the new particles grow to sizes that are active in cloud droplet formation. Although the gaseous precursors to Arctic marine SOA remain poorly defined, the measured levels of common continental SOA precursors (isoprene and monoterpenes) were low, whereas elevated mixing ratios of oxygenated volatile organic compounds (OVOCs) were inferred to arise via processes involving the sea surface microlayer. (3) The variability in the vertical distribution of black carbon (BC) under both springtime Arctic haze and more pristine summertime aerosol conditions was observed. Measured particle size distributions and mixing states were used to constrain, for the first time, calculations of aerosol–climate interactions under Arctic conditions. Aircraft- and ground-based measurements were used to better establish the BC source regions that supply the Arctic via long-range transport mechanisms, with evidence for a dominant springtime contribution from eastern and southern Asia to the middle troposphere, and a major contribution from northern Asia to the surface. (4) Measurements of ice nucleating particles (INPs) in the Arctic indicate that a major source of these particles is mineral dust, likely derived from local sources in the summer and long-range transport in the spring. In addition, INPs are abundant in the sea surface microlayer in the Arctic, and possibly play a role in ice nucleation in the atmosphere when mineral dust concentrations are low. (5) Amongst multiple aerosol components, BC was observed to have the smallest effective deposition velocities to high Arctic snow (0.03 cm s−1).
Abstract. Size-segregated aerosol sulfate concentrations were measured on board the Canadian Coast Guard Ship (CCGS) Amundsen in the Arctic during July 2014. The objective of this study was to utilize the isotopic composition of sulfate to address the contribution of anthropogenic and biogenic sources of aerosols to the growth of the different aerosol size fractions in the Arctic atmosphere. Non-seasalt sulfate is divided into biogenic and anthropogenic sulfate using stable isotope apportionment techniques. A considerable amount of the average sulfate concentration in the fine aerosols with a diameter < 0.49 µm was from biogenic sources (> 63 %), which is higher than in previous Arctic studies measuring above the ocean during fall (< 15 %) (Rempillo et al., 2011) and total aerosol sulfate at higher latitudes at Alert in summer (> 30 %) (Norman et al., 1999). The anthropogenic sulfate concentration was less than that of biogenic sulfate, with potential sources being long-range transport and, more locally, the Amundsen's emissions. Despite attempts to minimize the influence of ship stack emissions, evidence from larger-sized particles demonstrates a contribution from local pollution.A comparison of δ 34 S values for SO 2 and fine aerosols was used to show that gas-to-particle conversion likely occurred during most sampling periods. δ 34 S values for SO 2 and fine aerosols were similar, suggesting the same source for SO 2 and aerosol sulfate, except for two samples with a relatively high anthropogenic fraction in particles < 0.49 µm in diameter (15)(16)(17). The high biogenic fraction of sulfate fine aerosol and similar isotope ratio values of these particles and SO 2 emphasize the role of marine organisms (e.g., phytoplankton, algae, bacteria) in the formation of fine particles above the Arctic Ocean during the productive summer months.
<p><strong>Abstract.</strong> Size-segregated aerosol sulfate concentrations were measured on board the Canadian Coast Guard Ship (CCGS) Amundsen in the Arctic during July 2014. The objective of this study was to utilize the isotopic composition of sulfate to address the contribution of anthropogenic and biogenic sources of aerosols to the growth of the different aerosol size fractions in the Arctic atmosphere. Non-sea salt sulfate is divided into biogenic and anthropogenic sulfate using stable isotope apportionment techniques. A considerable amount of the average sulfate concentration in the fine aerosols with diameter < 0.49 &#956;m was from biogenic sources (> 70 %) which is higher than previous Arctic studies measuring above the ocean during fall (< 15 %) (Rempillo et al., 2011) and total aerosol sulfate at higher latitudes at Alert in summer (> 30 %) (Norman et al., 1999). The anthropogenic sulfate concentration was less than biogenic sulfate, with potential sources being long range transport and, more locally, the Amundsen&#8217;s emissions. Despite attempts to minimize the influence of ship stack emissions, evidence from larger-sized particles demonstrates a contribution from local pollution. A comparison of &#948;<sup>34</sup>S values for SO<sub>2</sub> and fine aerosols was used to show that gas-to-particle conversion likely occurred during most sampling periods. &#948;<sup>34</sup>S values for SO<sub>2</sub> and fine aerosols were similar suggesting the same source for SO<sub>2</sub> and aerosol sulfate, except for two samples with a relatively high anthropogenic fraction in particles < 0.49 &#956;m in diameter (July 15&#8211;17 and 17&#8211;19). The high biogenic fraction of sulfate fine aerosol and similar isotope ratio values of these particles and SO<sub>2</sub> emphasize the role of marine organisims (e.g. phytoplankton, algea, bacteria) in the formation of fine particles above the Arctic Ocean during the productive summer months.</p>
Abstract. Atmospheric dimethyl sulfide, DMS(g), is a climatically important sulfur compound and is the main source of biogenic sulfate aerosol in the Arctic atmosphere. DMS(g) production and emission to the atmosphere increase during the summer due to the greater ice-free sea surface and higher biological activity. We implemented DMS(g) in the Environment and Climate Change Canada’s (ECCC) online air quality forecast model, GEM-MACH (Global Environmental Multiscale–Modelling Air quality and CHemistry), and compared model simulations with DMS(g) measurements made in Baffin Bay and the Canadian Arctic Archipelago in July and August 2014. Two seawater DMS(aq) datasets were used as input for the simulations: (1) a DMS(aq) climatology dataset based on seawater concentration measurements (Lana et al., 2011) and (2) a DMS(aq) dataset based on satellite detection (Galí et al., 2018). In general, GEM-MACH simulations under-predict DMS(g) measurements, which is likely due to the negative biases in both DMS(aq) datasets. However, a higher correlation and smaller bias were obtained with the satellite dataset. Agreement with the observations improved when climatological values were replaced by DMS(aq) in situ values that were measured concurrently with atmospheric observations over Baffin Bay and the Lancaster Sound area in July 2014. The addition of DMS(g) to the GEM-MACH model resulted in a significant increase in atmospheric SO2 for some regions of the Canadian Arctic (up to 100 %). Analysis of the size-segregated sulfate aerosol in the model shows that a significant increase in sulfate mass occurs for particles with a diameter smaller than 200 nm due to the formation and growth of biogenic aerosol at high latitudes (>70∘ N). The enhancement in sulfate particles is most significant in the size range from 50 to 100 nm; however, this enhancement is stronger in the 200–1000 nm size range at lower latitudes (<70∘ N). These results emphasize the important role of DMS(g) in the formation and growth of fine and ultrafine sulfate-containing particles in the Arctic during the summertime.
Abstract. Vertical distributions of atmospheric dimethyl sulfide (DMS(g)) were sampled aboard the research aircraft Polar 6 near Lancaster
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