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Aerosols and clouds are key components of the marine atmosphere, impacting the Earth’s radiative budget with a net cooling effect over the industrial era that counterbalances greenhouse gas warming, yet with an uncertain amplitude. Here we report recent advances in our understanding of how open ocean aerosol sources are modulated by ocean biogeochemistry and how they, in turn, shape cloud coverage and properties. We organize these findings in successive steps from ocean biogeochemical processes to particle formation by nucleation and sea spray emissions, further particle growth by condensation of gases, the potential to act as cloud condensation nuclei or ice nucleating particles, and finally, their effects on cloud formation, optical properties, and life cycle. We discuss how these processes may be impacted in a warming climate and the potential for ocean biogeochemistry—climate feedbacks through aerosols and clouds.

 

Abstract Atmospheric gaseous elemental mercury (GEM) concentrations in the Arctic exhibit a clear summertime maximum, while the origin of this peak is still a matter of debate in the community. Based on summertime observations during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition and a modeling approach, we further investigate the sources of atmospheric Hg in the central Arctic. Simulations with a generalized additive model (GAM) show that long-range transport of anthropogenic and terrestrial Hg from lower latitudes is a minor contribution (~2%), and more than 50% of the explained GEM variability is caused by oceanic evasion. A potential source contribution function (PSCF) analysis further shows that oceanic evasion is not significant throughout the ice-covered central Arctic Ocean but mainly occurs in the Marginal Ice Zone (MIZ) due to the specific environmental conditions in that region. Our results suggest that this regional process could be the leading contributor to the observed summertime GEM maximum. In the context of rapid Arctic warming and the observed increase in width of the MIZ, oceanic Hg evasion may become more significant and strengthen the role of the central Arctic Ocean as a summertime source of atmospheric Hg. 

Abstract Chlorine radicals are strong atmospheric oxidants known to play an important role in the depletion of surface ozone and the degradation of methane in the Arctic troposphere. Initial oxidation processes of chlorine produce chlorine oxides, and it has been speculated that the final oxidation steps lead to the formation of chloric (HClO 3 ) and perchloric (HClO 4 ) acids, although these two species have not been detected in the atmosphere. Here, we present atmospheric observations of gas-phase HClO 3 and HClO 4 . Significant levels of HClO 3 were observed during springtime at Greenland (Villum Research Station), Ny-Ålesund research station and over the central Arctic Ocean, on-board research vessel Polarstern during the Multidisciplinary drifting Observatory for the Study of the Arctic Climate (MOSAiC) campaign, with estimated concentrations up to 7 × 10 6 molecule cm −3 . The increase in HClO 3 , concomitantly with that in HClO 4 , was linked to the increase in bromine levels. These observations indicated that bromine chemistry enhances the formation of OClO, which is subsequently oxidized into HClO 3 and HClO 4 by hydroxyl radicals. HClO 3 and HClO 4 are not photoactive and therefore their loss through heterogeneous uptake on aerosol and snow surfaces can function as a previously missing atmospheric sink for reactive chlorine, thereby reducing the chlorine-driven oxidation capacity in the Arctic boundary layer. Our study reveals additional chlorine species in the atmosphere, providing further insights into atmospheric chlorine cycling in the polar environment. 

The Arctic warms nearly four times faster than the global average, and aerosols play an increasingly important role in Arctic climate change. In the Arctic, sea salt is a major aerosol component in terms of mass concentration during winter and spring. However, the mechanisms of sea salt aerosol production remain unclear. Sea salt aerosols are typically thought to be relatively large in size but low in number concentration, implying that their influence on cloud condensation nuclei population and cloud properties is generally minor. Here we present observational evidence of abundant sea salt aerosol production from blowing snow in the central Arctic. Blowing snow was observed more than 20% of the time from November to April. The sublimation of blowing snow generates high concentrations of fine-mode sea salt aerosol (diameter below 300 nm), enhancing cloud condensation nuclei concentrations up to tenfold above background levels. Using a global chemical transport model, we estimate that from November to April north of 70° N, sea salt aerosol produced from blowing snow accounts for about 27.6% of the total particle number, and the sea salt aerosol increases the longwave emissivity of clouds, leading to a calculated surface warming of +2.30 W m⁻²under cloudy sky conditions.

 

Polar oceans and sea ice cover 15% of the Earth’s ocean surface, and the environment is changing rapidly at both poles. Improving knowledge on the interactions between the atmospheric and oceanic realms in the polar regions, a Surface Ocean–Lower Atmosphere Study (SOLAS) project key focus, is essential to understanding the Earth system in the context of climate change. However, our ability to monitor the pace and magnitude of changes in the polar regions and evaluate their impacts for the rest of the globe is limited by both remoteness and sea-ice coverage. Sea ice not only supports biological activity and mediates gas and aerosol exchange but can also hinder some in-situ and remote sensing observations. While satellite remote sensing provides the baseline climate record for sea-ice properties and extent, these techniques cannot provide key variables within and below sea ice. Recent robotics, modeling, and in-situ measurement advances have opened new possibilities for understanding the ocean–sea ice–atmosphere system, but critical knowledge gaps remain. Seasonal and long-term observations are clearly lacking across all variables and phases. Observational and modeling efforts across the sea-ice, ocean, and atmospheric domains must be better linked to achieve a system-level understanding of polar ocean and sea-ice environments. As polar oceans are warming and sea ice is becoming thinner and more ephemeral than before, dramatic changes over a suite of physicochemical and biogeochemical processes are expected, if not already underway. These changes in sea-ice and ocean conditions will affect atmospheric processes by modifying the production of aerosols, aerosol precursors, reactive halogens and oxidants, and the exchange of greenhouse gases. Quantifying which processes will be enhanced or reduced by climate change calls for tailored monitoring programs for high-latitude ocean environments. Open questions in this coupled system will be best resolved by leveraging ongoing international and multidisciplinary programs, such as efforts led by SOLAS, to link research across the ocean–sea ice–atmosphere interface.

 

Abstract The Arctic is warming faster than anywhere else on Earth, prompting glacial melt, permafrost thaw, and sea ice decline. These severe consequences induce feedbacks that contribute to amplified warming, affecting weather and climate globally. Aerosols and clouds play a critical role in regulating radiation reaching the Arctic surface. However, the magnitude of their effects is not adequately quantified, especially in the central Arctic where they impact the energy balance over the sea ice. Specifically, aerosols called ice nucleating particles (INPs) remain understudied yet are necessary for cloud ice production and subsequent changes in cloud lifetime, radiative effects, and precipitation. Here, we report observations of INPs in the central Arctic over a full year, spanning the entire sea ice growth and decline cycle. Further, these observations are size-resolved, affording valuable information on INP sources. Our results reveal a strong seasonality of INPs, with lower concentrations in the winter and spring controlled by transport from lower latitudes, to enhanced concentrations of INPs during the summer melt, likely from marine biological production in local open waters. This comprehensive characterization of INPs will ultimately help inform cloud parameterizations in models of all scales. 

Abstract Frequency and intensity of warm and moist air-mass intrusions into the Arctic have increased over the past decades and have been related to sea ice melt. During our year-long expedition in the remote central Arctic Ocean, a record-breaking increase in temperature, moisture and downwelling-longwave radiation was observed in mid-April 2020, during an air-mass intrusion carrying air pollutants from northern Eurasia. The two-day intrusion, caused drastic changes in the aerosol size distribution, chemical composition and particle hygroscopicity. Here we show how the intrusion transformed the Arctic from a remote low-particle environment to an area comparable to a central-European urban setting. Additionally, the intrusion resulted in an explosive increase in cloud condensation nuclei, which can have direct effects on Arctic clouds’ radiation, their precipitation patterns, and their lifetime. Thus, unless prompt actions to significantly reduce emissions in the source regions are taken, such intrusion events are expected to continue to affect the Arctic climate. 

Over a five-month time window between March and July 2020, scientists deployed two small uncrewed aircraft systems (sUAS) to the central Arctic Ocean as part of legs three and four of the MOSAiC expedition. These sUAS were flown to measure the thermodynamic and kinematic state of the lower atmosphere, including collecting information on temperature, pressure, humidity and winds between the surface and 1 km, as well as to document ice properties, including albedo, melt pond fraction, and open water amounts. The atmospheric state flights were primarily conducted by the DataHawk2 sUAS, which was operated primarily in a profiling manner, while the surface property flights were conducted using the HELiX sUAS, which flew grid patterns, profiles, and hover flights. In total, over 120 flights were conducted and over 48 flight hours of data were collected, sampling conditions that included temperatures as low as −35 °C and as warm as 15 °C, spanning the summer melt season.

 

Abstract Despite the key role of the Arctic in the global Earth system, year-round in-situ atmospheric composition observations within the Arctic are sparse and mostly rely on measurements at ground-based coastal stations. Measurements of a suite of in-situ trace gases were performed in the central Arctic during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition. These observations give a comprehensive picture of year-round near-surface atmospheric abundances of key greenhouse and trace gases, i.e., carbon dioxide, methane, nitrous oxide, ozone, carbon monoxide, dimethylsulfide, sulfur dioxide, elemental mercury, and selected volatile organic compounds (VOCs). Redundancy in certain measurements supported continuity and permitted cross-evaluation and validation of the data. This paper gives an overview of the trace gas measurements conducted during MOSAiC and highlights the high quality of the monitoring activities. In addition, in the case of redundant measurements, merged datasets are provided and recommended for further use by the scientific community. 

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 (<5 m s−1) and shallow PBL (<50 m), the 7-day mean dry deposition removal rate can reach up to 1.0 ppb h−1. Our study highlights the importance of an accurate description of dry deposition to Arctic sea ice in models to quantify the current and future O3 sink in the Arctic, impacting the tropospheric O3 budget, which has been modified in the last century largely due to anthropogenic activities.