Abstract. The sea-surface microlayer and bulk seawater can contain ice-nucleating particles (INPs) and these INPs can be emitted into the atmosphere. Our current understanding of the properties, concentrations, and spatial and temporal distributions of INPs in the microlayer and bulk seawater is limited. In this study we investigate the concentrations and properties of INPs in microlayer and bulk seawater samples collected in the Canadian Arctic during the summer of 2014. INPs were ubiquitous in the microlayer and bulk seawater with freezing temperatures in the immersion mode as high as −14 • C. A strong negative correlation (R = −0.7, p = 0.02) was observed between salinity and freezing temperatures (after correction for freezing depression by the salts). One possible explanation is that INPs were associated with melting sea ice. Heat and filtration treatments of the samples show that the INPs were likely heat-labile biological materials with sizes between 0.02 and 0.2 µm in diameter, consistent with previous measurements off the coast of North America and near Greenland in the Arctic. The concentrations of INPs in the microlayer and bulk seawater were consistent with previous measurements at several other locations off the coast of North America. However, our average microlayer concentration was lower than previous observations made near Greenland in the Arctic. This difference could not be explained by chlorophyll a concentrations derived from satellite measurements. In addition, previous studies found significant INP enrichment in the microlayer, relative to bulk seawater, which we did not observe in this study. While further studies are needed to understand these differences, we confirm that there is a source of INP in the microlayer and bulk seawater in the Canadian Arctic that may be important for atmospheric INP concentrations.
This study presents temporal variations in concentrations of chlorophyll a (Chl a), particulate and dissolved dimethylsulfoniopropionate (DMSPp and DMSPd) in the sea ice and underlying water column in the Canadian Arctic Archipelago during the spring of 2010 and 2011. During both years, bottom ice Chl a, DMSPp and DMSPd concentrations were high (up to 1328 mg L 21, 15,082 nmol L 21, and 6110 nmol L 21 , respectively) in May and decreased thereafter. The release of bottom ice algae and DMSPp in the water column was gradual in 2010 and rapid (8 days) in 2011. Bottom brine drainage during the presnowmelt period in 2010 and a rapid loss of the snow cover in 2011 coinciding with rain events explain most of the difference between the 2 years. During both years, less than 13% of the DMSPd lost from the ice was detected in the water column, suggesting a rapid microbial consumption. An under-ice diatom bloom developed in both years. In 2010, the bloom was dominated by centric diatoms while in 2011 pennates dominated, likely reflecting seeding by ice algae following the faster snowmelt progression induced by rainfall events in 2011. Both under-ice blooms were associated with high DMSPp concentrations (up to 185 nmol L 21 ), but pennate diatoms showed DMSPp/Chl a ratios twice higher than centrics. These results highlight the key role of snowmelt and precipitation on the temporal pattern of ice-DMSP release to the water column and on the timing, taxonomic composition, and DMSP content of phytoplankton under-ice blooms in the Arctic.
International audienceDimethyl sulfide (DMS) plays a major role in the global sulfur cycle. In addition, its atmospheric oxidation products contribute to the formation and growth of atmospheric aerosol particles, thereby influencing cloud condensation nuclei (CCN) populations and thus cloud formation. The pristine summertime Arctic atmosphere is strongly influenced by DMS. However, atmospheric DMS mixing ratios have only rarely been measured in the summertime Arctic. During July-August, 2014, we conducted the first high time resolution (10 Hz) DMS mixing ratio measurements for the eastern Canadian Archipelago and Baffin Bay as one component of the Network on Climate and Aerosols: Addressing Key Uncertainties in Remote Canadian Environments (NETCARE). DMS mixing ratios ranged from below the detection limit of 4 to 1155 pptv (median 186 pptv) during the 21-day shipboard campaign. A transfer velocity parameterization from the literature coupled with coincident atmospheric and seawater DMS measurements yielded air-sea DMS flux estimates ranging from 0.02 to 12 µmol m-2 d-1. Air-mass trajectory analysis using FLEXPART-WRF and sensitivity simulations with the GEOS-Chem chemical transport model indicated that local sources (Lancaster Sound and Baffin Bay) were the dominant contributors to the DMS measured along the 21-day ship track, with episodic transport from the Hudson Bay System. After adjusting GEOS-Chem oceanic DMS values in the region to match measurements, GEOS-Chem reproduced the major features of the measured time series but was biased low overall (2-1006 pptv, median 72 pptv), although within the range of uncertainty of the seawater DMS source. However, during some 1-2 day periods the model underpredicted the measurements by more than an order of magnitude. Sensitivity tests indicated that non-marine sources (lakes, biomass burning, melt ponds, and coastal tundra) could make additional episodic contributions to atmospheric DMS in the study region, although local marine sources of DMS dominated. Our results highlight the need for both atmospheric and seawater DMS data sets with greater spatial and temporal resolution, combined with further investigation of non-marine DMS sources for the Arctic
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. The source strength and capability of aerosol particles in the Arctic to act as cloud condensation nuclei have important implications for understanding the indirect aerosolcloud effect within the polar climate system. It has been shown in several Arctic regions that ultrafine particle (UFP) formation and growth is a key contributor to aerosol number concentrations during the summer. This study uses aerosol number size distribution measurements from shipboard expeditions aboard the research icebreaker CCGS Amundsen in the summers of 2014 and 2016 throughout the Canadian Arctic to gain a deeper understanding of the drivers of UFP formation and growth within this marine boundary layer. UFP number concentrations (diameter > 4 nm) in the range of 10 1 -10 4 cm −3 were observed during the two seasons, with concentrations greater than 10 3 cm −3 occurring more frequently in 2016. Higher concentrations in 2016 were associated with UFP formation and growth, with events occurring on 41 % of days, while events were only observed on 6 % of days in 2014. Assessment of relevant parameters for aerosol nucleation showed that the median condensation sink in this region was approximately 1.2 h −1 in 2016 and 2.2 h −1 in 2014, which lie at the lower end of ranges observed at even the most remote stations reported in the literature. Apparent growth rates of all observed events in both expeditions averaged 4.3 ± 4.1 nm h −1 , in general agreement with other recent studies at similar latitudes. Higher solar radiation, lower cloud fractions, and lower sea ice concentrations combined with differences in the developmental stage and activity of marine microbial communities within the Canadian Arctic were documented and help explain differences between the aerosol measurements made during the 2014 and 2016 expeditions. These findings help to motivate further studies of biosphere-atmosphere interactions within the Arctic marine environment to explain the production of UFP and their growth to sizes relevant for cloud droplet activation.
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