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Coccolithophores are typically thought of as photoautotrophs, yet a few genera inhabit sub-euphotic environments with insufficient light for photosynthesis, suggesting that other carbon acquisition strategies are likely. Field experiments were performed in the northwest Atlantic (a region with potentially abundant coccolithophores). Phytoplankton populations were incubated with 14 C-labeled dissolved organic carbon (DOC) compounds, acetate, mannitol, and glycerol. Coccolithophores were sorted from these populations 24 hours later using flow cytometry, and DOC uptake was measured. DOC uptake rates were as high as 10 −15 moles cell −1 day −1 , slow relative to photosynthesis rates (10 −12 moles cell −1 day −1 ). Growth rates on the organic compounds were low, suggesting that osmotrophy plays more of a survival strategy in low-light situations. Assimilated DOC was found in both particulate organic carbon and calcite coccoliths (particulate inorganic carbon), suggesting that osmotrophic uptake of DOC into coccolithophore calcite is a small but notable part of the biological carbon pump and alkalinity pump paradigms.

Dry deposition to the surface is one of the main removal pathways of tropospheric ozone (O3). We quantified for the first time the impact of O3 deposition to the Arctic sea ice on the planetary boundary layer (PBL) O3 concentration and budget using year-round flux and concentration observations from the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) campaign and simulations with a single-column atmospheric chemistry and meteorological model (SCM). Based on eddy-covariance O3 surface flux observations, we find a median surface resistance on the order of 20,000 s m−1, resulting in a dry deposition velocity of approximately 0.005 cm s−1. This surface resistance is up to an order of magnitude larger than traditionally used values in many atmospheric chemistry and transport models. The SCM is able to accurately represent the yearly cycle, with maxima above 40 ppb in the winter and minima around 15 ppb at the end of summer. However, the observed springtime ozone depletion events are not captured by the SCM. In winter, the modelled PBL O3 budget is governed by dry deposition at the surface mostly compensated by downward turbulent transport of O3 towards the surface. Advection, which is accounted for implicitly by nudging to reanalysis data, poses a substantial, mostly negative, contribution to the simulated PBL O3 budget in summer. During episodes with low wind speed (

Near-surface mercury and ozone depletion events occur in the lowest part of the atmosphere during Arctic spring. Mercury depletion is the first step in a process that transforms long-lived elemental mercury to more reactive forms within the Arctic that are deposited to the cryosphere, ocean, and other surfaces, which can ultimately get integrated into the Arctic food web. Depletion of both mercury and ozone occur due to the presence of reactive halogen radicals that are released from snow, ice, and aerosols. In this work, we added a detailed description of the Arctic atmospheric mercury cycle to our recently published version of the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem 4.3.3) that includes Arctic bromine and chlorine chemistry and activation/recycling on snow and aerosols. The major advantage of our modelling approach is the online calculation of bromine concentrations and emission/recycling that is required to simulate the hourly and daily variability of Arctic mercury depletion. We used this model to study coupling between reactive cycling of mercury, ozone, and bromine during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) spring season in 2020 and evaluated results compared to land-based, ship-based, and remote sensing observations. The model predicts that elemental mercury oxidation is driven largely by bromine chemistry and that particulate mercury is the major form of oxidized mercury. The model predicts that the majority (74%) of oxidized mercury deposited to land-based snow is re-emitted to the atmosphere as gaseous elemental mercury, while a minor fraction (4%) of oxidized mercury that is deposited to sea ice is re-emitted during spring. Our work demonstrates that hourly differences in bromine/ozone chemistry in the atmosphere must be considered to capture the springtime Arctic mercury cycle, including its integration into the cryosphere and ocean.

6 pags., 2 figs., Unlike bromine, the effect of iodine chemistry on the Arctic surface ozone budget is poorly constrained. We present ship-based measurements of halogen oxides in the high Arctic boundary layer from the sunlit period of March to October 2020 and show that iodine enhances springtime tropospheric ozone depletion. We find that chemical reactions between iodine and ozone are the second highest contributor to ozone loss over the study period, after ozone photolysis-initiated loss and ahead of bromine., This study received funding from the European Research Council Executive Agency under the European Union’s Horizon 2020 Research and Innovation Program (project ERC‐2016‐COG 726349 CLIMAHAL and ERC-2016-STG 714621 GASPARCON) and the European Commission via the EMME-CARE project and was supported by the Consejo Superior de Investigaciones Científicas of Spain. This work was supported by the European Union’s Horizon 2020 Research and Innovation Programme under grant agreement no. 856612 and the Academy of Finland (project no. 334514). The Indian Institute of Tropical Meteorology is funded by the Ministry of Earth Sciences, Government of India. Ozone, CO, CH4 and AMS measurements were funded by the Swiss National Science Foundation (grant 200021_188478), the Swiss Polar Institute and U.S. National Science Foundation grants 1914781 and 1807163. J.S. holds the Ingvar Kamprad chair for extreme environments research, sponsored by Ferring Pharmaceuticals. Data reported in this manuscript were produced as part of the international MOSAiC expedition with tag MOSAiC20192020, with activities supported by Polarstern expedition AWI-PS122_00. H.S. was funded by the European ERA-PLANET projects iGOSP and iCUPE (consortium agreement no. 689443 for both projects). We thank FORMAS and the Swedish Polar Research Secretariat for support. We gratefully acknowledge funding by the Deutsche Forschungsgemeinschaft (project no. 268020496 – TRR 172) within the Transregional Collaborative Research Center ‘ArctiC Amplification: Climate Relevant Atmospheric and SurfaCe Processes, and Feedback Mechanisms (AC)3’ in subproject C03. We thank I. Bourgeois (NOAA/CIRES) for providing the ATom NOx data.

The methylamines form part of the marine organic nitrogen pool. Although they are ubiquitous in marine systems, little is known about their distribution, production and fate in the marine environment. Analytical methods have been developed for their analysis in marine waters, but these have employed custom-made apparatus, limiting data to a few studies. Here, we report a method developed for the determination of methylamines in seawater which combines headspace solid phase micro-extraction (SPME) and gas chromatography with selective nitrogen detection. Gaseous methylamines were pre-concentrated from water samples (approximately 1 L) heated to 60 oC, onto a polydimethylsiloxane/divinylbenzene SPME fibre located in the headspace of the extraction flask. The analytes were then thermally desorbed from the fibre in a gas chromatograph containing a CP-Volamine column and a nitrogen-phosphorus detector. The method was routinely calibrated down to 1 nM for all three analytes using matrix-matched external standards. Limits of detection were determined operationally and ranged from 0.4-2.9 nM during two sampling campaigns. The analytes were detected in seawater samples from the English Channel and Southern Ocean where concentrations up to 20 and 5.6 nM were measured, respectively, consistent with previously reported levels. We propose this method for the analysis of methylamines, and other low molecular weight amines, as it is sensitive, robust, and the necessary equipment is widely-available.

Predictions of the ocean-atmosphere flux of dimethyl sulfide will be improved by understanding what controls seasonal and regional variations in dimethylsulfoniopropionate (DMSP) production. To investigate the influence of high levels of irradiance including ultraviolet radiation (UVR), on DMSP synthesis rates (mu DMSP) and inorganic carbon fixation (mu POC) by natural phytoplankton communities, nine experiments were carried out at different locations in the low nutrient, high light environment of the northeastern Tropical Atlantic. Rates of mu DMSP and mu POC were determined by measuring the incorporation of inorganic C-13 into DMSP and particulate organic carbon. Based on measurements over discrete time intervals during the day, a unique mu DMSP vs. irradiance (P vs. E) relationship was established. Comparison is made with the P vs. E relationship for mu POC, indicating that light saturation of DMSP occurs at similar irradiance to mu POC and is closely coupled to carbon fixation on a diel basis. Photoinhibition during the middle of the day was exacerbated by exposure to UVR, causing an additional 55-60% inhibition of both mu DMSP and mu POC at the highest light levels. In addition, decreased production of DMSP in response to UVR-induced photoxidative stress, contrasted with the increased net synthesis of photoprotective xanthophyll pigments. Together these results indicate that DMSP production by phytoplankton in the tropical ocean is not regulated in the short term by the necessity to control increasing photooxidative stress as irradiance increases during the day. The study provides new insight into the regulation of resource allocation into this biogeochemically important, multi-functional compatible solute.

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.

Long-term time series data show that ocean acidification is occurring in the subtropical oceans. As a component of an in situ mesocosm experiment carried out off Gran Canaria in the subtropical North Atlantic, we examined the influence of ocean acidification on the net production of dimethylsulfide (DMS). Over 23 days under oligotrophic conditions, time-integrated DMS concentrations showed an inverse relationship of −0.21 ± 0.02 nmol DMS nmol−1 H+ across the gradient of H+ concentration of 8.8–23.3 nmol l−1, equivalent to a range of pCO2 of 400–1,252 atm. Proportionally similar decreases in the concentrations of both dissolved and particulate dimethylsulfoniopropionate (DMSP) were observed in relation to increasing H+ concentration between the mesocosms. The reduced net production of DMSP with increased acidity appeared to result from a decrease in abundance of a DMSP-rich nanophytoplankton population. A 35S-DMSP tracer approach was used to determine rates of dissolved DMSP catabolism, including DMS production, across the mesocosm treatments. Over a phase of increasing DMS concentrations during the experiment, the specific rates of DMS production were significantly reduced at elevated H+ concentration. These rates were closely correlated to the rates of net DMS production indicating that transformation of dissolved DMSP to DMS by bacteria was a major component of DMS production. It was not possible to resolve whether catabolism of DMSP was directly influenced by H+ concentrations or was an indirect response in the bacterial community composition associated with reduced DMSP availability. There is a pressing need to understand how subtropical planktonic communities respond to the predicted gradual prolonged ocean acidification, as alterations in the emission of DMS from the vast subtropical oceans could influence atmospheric chemistry and potentially climate, over a large proportion of the Earth's surface.

The coccolithophore Emiliania huxleyi forms some of the largest phytoplankton blooms in the ocean. The rapid demise of these blooms has been linked to viral infections. E. huxleyi abundance, distribution, and nutritional status make them an important food source for the heterotrophic protists which are classified as microzooplankton in marine food webs. In this study we investigated the fate of E. huxleyi (CCMP 374) infected with virus strain EhV-86 in a simple predator-prey interaction. The ingestion rates of Oxyrrhis marina were significantly lower (between 26.9 and 50.4%) when fed virus-infected E. huxleyi cells compared to non-infected cells. Despite the lower ingestion rates, O. marina showed significantly higher growth rates (between 30 and 91.3%) when fed infected E. huxleyi cells, suggesting higher nutritional value and/or greater assimilation of infected E. huxleyi cells. No significant differences were found in O. marina cell volumes or fatty acids profiles. These results show that virally infected E. huxleyi support higher growth rates of single celled heterotrophs and in addition to the “viral shunt” hypothesis, viral infections may also divert more carbon to mesozooplankton grazers.

The coccolithophore Emiliania huxleyi forms some of the largest phytoplankton blooms in the ocean. The rapid demise of these blooms has been linked to viral infections. E. huxleyi abundance, distribution, and nutritional status make them an important food source for the heterotrophic protists which are classified as microzooplankton in marine food webs. In this study we investigated the fate of E. huxleyi (CCMP 374) infected with virus strain EhV-86 in a simple predator-prey interaction. The ingestion rates of Oxyrrhis marina were significantly lower (between 26.9 and 50.4%) when fed virus-infected E. huxleyi cells compared to non-infected cells. Despite the lower ingestion rates, O. marina showed significantly higher growth rates (between 30 and 91.3%) when fed infected E. huxleyi cells, suggesting higher nutritional value and/or greater assimilation of infected E. huxleyi cells. No significant differences were found in O. marina cell volumes or fatty acids profiles. These results show that virally infected E. huxleyi support higher growth rates of single celled heterotrophs and in addition to the “viral shunt” hypothesis, viral infections may also divert more carbon to mesozooplankton grazers.

Emissions of dimethylsulfide (DMS) from the polar oceans play a key role in atmospheric processes and climate. Therefore, it is important we increase our understanding of how DMS production in these regions may respond to environmental change. The polar oceans are particularly vulnerable to ocean acidification (OA). However, our understanding of the polar DMS response is limited to two studies conducted in Arctic waters, where in both cases DMS concentrations decreased with increasing acidity. Here, we report on our findings from seven summertime shipboard microcosm experiments undertaken in a variety of locations in the Arctic Ocean and Southern Ocean. These experiments reveal no significant effects of short term OA on the net production of DMS by planktonic communities. This is in contrast to identical experiments from temperate NW European shelf waters where surface ocean communities responded to OA with significant increases in dissolved DMS concentrations. A meta-analysis of the findings from both temperate and polar waters (n = 18 experiments) reveals clear regional differences in the DMS response to OA. We suggest that these regional differences in DMS response reflect the natural variability in carbonate chemistry to which the respective communities may already be adapted. Future temperate oceans could be more sensitive to OA resulting in a change in DMS emissions to the atmosphere, whilst perhaps surprisingly DMS emissions from the polar oceans may remain relatively unchanged. By demonstrating that DMS emissions from geographically distinct regions may vary in response to OA, our results may facilitate a better understanding of Earth's future climate. Our study suggests that the way in which processes that generate DMS respond to OA may be regionally distinct and this should be taken into account in predicting future DMS emissions and their influence on Earth's climate.

© 2015, The Oceanography Society. All rights reserved. Ocean acidification (OA) research seeks to understand how marine ecosystems and global elemental cycles will respond to changes in seawater carbonate chemistry in combination with other environmental perturbations such as warming, eutrophication, and deoxygenation. Here, we discuss the effectiveness and limitations of current research approaches used to address this goal. A diverse combination of approaches is essential to decipher the consequences of OA to marine organisms, communities, and ecosystems. Consequently, the benefits and limitations of each approach must be considered carefully. Major research challenges involve experimentally addressing the effects of OA in the context of large natural variability in seawater carbonate system parameters and other interactive variables, integrating the results from different research approaches, and scaling results across different temporal and spatial scales.