Surface ocean biogeochemistry and photochemistry regulate ocean–atmosphere fluxes of trace gases critical for Earth's atmospheric chemistry and climate. The oceanic processes governing these fluxes are often sensitive to the changes in ocean pH (or p CO 2 ) accompanying ocean acidification (OA), with potential for future climate feedbacks. Here, we review current understanding (from observational, experimental and model studies) on the impact of OA on marine sources of key climate-active trace gases, including dimethyl sulfide (DMS), nitrous oxide (N 2 O), ammonia and halocarbons. We focus on DMS, for which available information is considerably greater than for other trace gases. We highlight OA-sensitive regions such as polar oceans and upwelling systems, and discuss the combined effect of multiple climate stressors (ocean warming and deoxygenation) on trace gas fluxes. To unravel the biological mechanisms responsible for trace gas production, and to detect adaptation, we propose combining process rate measurements of trace gases with longer term experiments using both model organisms in the laboratory and natural planktonic communities in the field. Future ocean observations of trace gases should be routinely accompanied by measurements of two components of the carbonate system to improve our understanding of how in situ carbonate chemistry influences trace gas production. Together, this will lead to improvements in current process model capabilities and more reliable predictions of future global marine trace gas fluxes.
Phytoplankton blooms in the Arctic marginal ice zone (MIZ) can be prolific dimethylsulfide (DMS) producers, thereby influencing regional aerosol formation and cloud radiative forcing. Here we describe the distribution of DMS and its precursor dimethylsulfoniopropionate (DMSP) across the Baffin Bay receding ice edge in early summer 2016. Overall, DMS and total DMSP (DMSPt) increased towards warmer waters of Atlantic origin concurrently with more advanced ice-melt and bloom stages. Relatively high DMS and DMSPt (medians of 6.3 and 70 nM, respectively) were observed in the surface layer (0–9 m depth), and very high values (reaching 74 and 524 nM, respectively) at the subsurface biomass maximum (15–30 m depth). Microscopic and pigment analyses indicated that subsurface DMS and DMSPt peaks were associated with Phaeocystis pouchetii, which bloomed in Atlantic-influenced waters and reached unprecedented biomass levels in Baffin Bay. In surface waters, DMS concentrations and DMS:DMSPt ratios were higher in the MIZ (medians of 12 nM and 0.15, respectively) than in fully ice-covered or ice-free conditions, potentially associated with enhanced phytoplanktonic DMSP release and bacterial DMSP cleavage (high dddP:dmdA gene ratios). Mean sea–air DMS fluxes (µmol m–2 d–1) increased from 0.3 in ice-covered waters to 10 in open waters (maximum of 26) owing to concurrent trends in near-surface DMS concentrations and physical drivers of gas exchange. Using remotely sensed sea-ice coverage and a compilation of sea–air DMS flux data, we estimated that the pan-Arctic DMS emission from the MIZ (EDMS, MIZ) was 5–13 Gg S yr–1. North of 80°N, EDMS, MIZ might have increased by around 10 ± 4% yr–1 between 2003 and 2014, likely exceeding open-water emissions in June and July. We conclude that EDMS, MIZ must be taken into account to evaluate plankton-climate feedbacks in the Arctic.
<p><strong>Abstract.</strong> The source strength and capability of aerosol particles in the Arctic to act as cloud condensation nuclei have important implications for understanding the indirect aerosol-cloud 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 ship-board measurement expeditions aboard the research icebreaker CCGS <i>Amundsen</i> 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&#8201;>&#8201;4&#8201;nm) in the range of 10<sup>1</sup>&#8211;10<sup>4</sup>&#8201;cm<sup>&#8722;3</sup> were observed across the two seasons, with concentrations greater than 10<sup>3</sup>&#8201;cm<sup>&#8722;3</sup> occurring more frequently in 2016. Higher concentrations in 2016 were associated with UFP formation and growth, with events occurring on 41&#8201;% of days, while events were only observed on 6&#8201;% of days in 2014. Assessment of relevant parameters for aerosol nucleation showed that the median condensation sink in this region was approximately 1.2&#8201;h<sup>&#8722;1</sup> in 2016 and 2.2&#8201;h<sup>&#8722;1</sup> 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&#8201;&#177;&#8201;4.1&#8201;nm&#8201;h<sup>&#8722;1</sup>, 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.</p>
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