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Sea spray aerosol (SSA) particles strongly influence clouds and climate but the potential impact of ocean microbiota on SSA fluxes is still a matter of active research. Here–by means of in situ ship-borne measurements–we explore simultaneously molecular-level chemical properties of organic matter (OM) in oceans, sea ice, and the ambient PM2.5 aerosols along a transect of 15,000 km from the western Pacific Ocean (36°13′N) to the Southern Ocean (75°15′S). By means of orbitrap mass spectrometry and optical characteristics, lignin-like material (24 ± 5 %) and humic material (57 ± 8 %) were found to dominate the pelagic Pacific Ocean surface, while intermediate conditions were observed in the Pacific-Southern Ocean waters. In the marine atmosphere, we found a gradient of features in the aerosol: lignin-like material (31 ± 9 %) dominating coastal areas and the pelagic Pacific Ocean, whereas lipid-like (23 ± 16 %) and protein-like (11 ± 10 %) OM controlled the sympagic Southern Ocean (sea ice-influence). The results of this study showed that the OM composition in the ocean, which changes with latitude, affects the OM in aerosol compositions in the atmosphere. This study highlights the importance of the global-scale OM monitoring of the close interaction between the ocean, sea ice, and the atmosphere. Sympagic primary marine aerosols in polar regions must be treated differently from other pelagic-type oceans

Dimethyl sulfide (DMS) produced by marine algae represents the largest natural emission of sulfur to the atmosphere. The oxidation of DMS is a key process affecting new particle formation that contributes to the radiative forcing of the Earth. In this study, atmospheric DMS and its major oxidation products (methanesulfonic acid, MSA; non-sea-salt sulfate, nss-SO42-) and particle size distributions were measured at King Sejong station located in the Antarctic Peninsula during the austral spring-summer period in 2018-2020. The observatory was surrounded by open ocean and first-year and multi-year sea ice. Importantly, oceanic emissions and atmospheric oxidation of DMS showed distinct differences depending on source regions. A high mixing ratio of atmospheric DMS was observed when air masses were influenced by the open ocean and first-year sea ice due to the abundance of DMS producers such as pelagic phaeocystis and ice algae. However, the concentrations of MSA and nss-SO42- were distinctively increased for air masses originating from first-year sea ice as compared to those originating from the open ocean and multi-year sea ice, suggesting additional influences from the source regions of atmospheric oxidants. Heterogeneous chemical processes that actively occur over first-year sea ice tend to accelerate the release of bromine monoxide (BrO), which is the most efficient DMS oxidant in Antarctica. Model-estimates for surface BrO confirmed that high BrO mixing ratios were closely associated with first-year sea ice, thus enhancing DMS oxidation. Consequently, the concentration of newly formed particles originated from first-year sea ice, which was a strong source area for both DMS and BrO was greater than from open ocean (high DMS but low BrO). These results indicate that first-year sea ice plays an important yet overlooked role in DMS-induced new particle formation in polar environments, where warming-induced sea ice changes are pronounced.

Oceanic dimethyl sulfide (DMS) emissions have been recognized as a biological regulator of climate by contributing to cloud formation. Despite decades of research, the climatic role of DMS remains ambiguous largely because of limited observational evidence for DMS-induced cloud condensation nuclei (CCN) enhancement. Here, we report concurrent measurement of DMS, physiochemical properties of aerosol particles, and CCN in the Arctic atmosphere during the phytoplankton bloom period of 2010. We encountered multiple episodes of new particle formation (NPF) and particle growth when DMS mixing ratios were both low and high. The growth of particles to sizes at which they can act as CCN accelerated in response to an increase in atmospheric DMS. Explicitly, the sequential increase in all relevant parameters (including the source rate of condensable vapor, the growth rate of particles, Aitken mode particles, hygroscopicity, and CCN) was pronounced at the DMS-derived NPF and particle growth events. This field study unequivocally demonstrates the previously unconfirmed roles of DMS in the growth of particles into climate-relevant size and eventual CCN activation.

There are few shipborne observations addressing the factors influencing the relationships of the formation and growth of aerosol particles with cloud condensation nuclei (CCN) in remote marine environments. In this study, the physical properties of aerosol particles throughout the Arctic Ocean and Pacific Ocean were measured aboard the Korean icebreaker R/V Araon during the summer of 2017 for 25 d. A number of new particle formation (NPF) events and growth were frequently observed in both Arctic terrestrial and Arctic marine air masses. By striking contrast, NPF events were not detected in Pacific marine air masses. Three major aerosol categories are therefore discussed: (1) Arctic marine (aerosol number concentration CN2.5: 413±442 cm−3), (2) Arctic terrestrial (CN2.5: 1622±1450 cm−3) and (3) Pacific marine (CN2.5: 397±185 cm−3), following air mass back-trajectory analysis. A major conclusion of this study is not only that the Arctic Ocean is a major source of secondary aerosol formation relative to the Pacific Ocean but also that open-ocean sympagic and terrestrially influenced coastal ecosystems both contribute to shaping aerosol size distributions. We suggest that terrestrial ecosystems – including river outflows and tundra – strongly affect aerosol emissions in the Arctic coastal areas, possibly more than anthropogenic Arctic emissions. The increased river discharge, tundra emissions and melting sea ice should be considered in future Arctic atmospheric composition and climate simulations. The average CCN concentrations at a supersaturation ratios of 0.4 % were 35±40 cm−3, 71±47 cm−3 and 204±87 cm−3 for Arctic marine, Arctic terrestrial and Pacific marine aerosol categories, respectively. Our results aim to help evaluate how anthropogenic and natural atmospheric sources and processes affect the aerosol composition and cloud properties