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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).

Concentrations and δ34S values for SO2 and size-segregated sulfate aerosols were determined for air monitoring station 13 (AMS 13) at Fort MacKay in the Athabasca oil sands region, northeastern Alberta, Canada as part of the Joint Canada-Alberta Implementation Plan for Oil Sands Monitoring (JOSM) campaign from 13 August to 5 September 2013. Sulfate aerosols and SO2 were collected on filters using a high-volume sampler, with 12 or 24 h time intervals. Sulfur dioxide (SO2) enriched in 34S was exhausted by a chemical ionization mass spectrometer (CIMS) operated at the measurement site and affected isotope samples for a portion of the sampling period. It was realized that this could be a useful tracer and samples collected were divided into two sets. The first set includes periods when the CIMS was not running (CIMS-OFF) and no 34SO2 was emitted. The second set is for periods when the CIMS was running (CIMS-ON) and 34SO2 was expected to affect SO2 and sulfate high-volume filter samples. δ34S values for sulfate aerosols with diameter D > 0.49 µm during CIMS-OFF periods (no tracer 34SO2 present) indicate the sulfur isotope characteristics of secondary sulfate in the region. Such aerosols had δ34S values that were isotopically lighter (down to −5.3 ‰) than what was expected according to potential sulfur sources in the Athabasca oil sands region (+3.9 to +11.5 ‰). Lighter δ34S values for larger aerosol size fractions are contrary to expectations for primary unrefined sulfur from untreated oil sands (+6.4 ‰) mixed with secondary sulfate from SO2 oxidation and accompanied by isotope fractionation in gas phase reactions with OH or the aqueous phase by H2O2 or O3. Furthermore, analysis of 34S enhancements of sulfate and SO2 during CIMS-ON periods indicated rapid oxidation of SO2 from this local source at ground level on the surface of aerosols before reaching the high-volume sampler or on the collected aerosols on the filters in the high-volume sampler. Anti-correlations between δ34S values of dominantly secondary sulfate aerosols with D r = −0.80 and r = −0.76, respectively) were observed, suggesting that SO2 was oxidized by a transition metal ion (TMI) catalyzed pathway involving O2 and Fe3+ and/or Mn2+, an oxidation pathway known to favor lighter sulfur isotopes. Correlations between SO2 to sulfate conversion ratio (F(s)) and the concentrations of α-pinene (r = 0.85), β-pinene (r = 0.87), and limonene (r = 0.82) during daytime suggests that SO2 oxidation by Criegee biradicals may be a potential oxidation pathway in the study region.