Arctic Primary Aerosol Production Strongly Influenced by Riverine Organic Matter.

The sources of primary and secondary aerosols in the Arctic are still poorly known. A number of surface seawater samples-with varying degrees of Arctic riverine and sea ice influences-were used in a sea spray generation chamber to test them for their potential to produce sea spray aerosols (SSA) and cloud condensation nuclei (CCN). Our interdisciplinary data showed that both sea salt and organic matter (OM) significantly influenced the SSA production. The number concentration of SSA in the coastal samples was negatively correlated with salinity and positively correlated with a number of OM tracers, including dissolved and chromophoric organic carbon (DOC, CDOM), marine microgels and chlorophyll a (Chl-a) but not for viral and bacterial abundances; indicating that OM of riverine origin enhances primary aerosol production. When all samples were considered, transparent exopolymer particles (TEP) were found to be the best indicator correlating positively with the ratio number concentration of SSA/salinity. CCN efficiency was not observed to differ between the SSA from the various samples, despite differences in organic characteristics. It is suggested that the large amount of freshwater from river runoff have a substantial impact on primary aerosols production mechanisms, possibly affecting the cloud radiative forcing.

Comparison of Hygroscopicity, Volatility, and Mixing State of Submicrometer Particles between Cruises over the Arctic Ocean and the Pacific Ocean.

Ship-borne measurements of ambient aerosols were conducted during an 11 937 km cruise over the Arctic Ocean (cruise 1) and the Pacific Ocean (cruise 2). A frequent nucleation event was observed during cruise 1 under marine influence, and the abundant organic matter resulting from the strong biological activity in the ocean could contribute to the formation of new particles and their growth to a detectable size. Concentrations of particle mass and black carbon increased with increasing continental influence from polluted areas. During cruise 1, multiple peaks of hygroscopic growth factor (HGF) of 1.1-1.2, 1.4, and 1.6 were found, and higher amounts of volatile organic species existed in the particles compared to that during cruise 2, which is consistent with the greater availability of volatile organic species caused by the strong oceanic biological activity (cruise 1). Internal mixtures of volatile and nonhygroscopic organic species, nonvolatile and less-hygroscopic organic species, and nonvolatile and hygroscopic nss-sulfate with varying fractions can be assumed to constitute the submicrometer particles. On the basis of elemental composition and morphology, the submicrometer particles were classified into C-rich mixture, S-rich mixture, C/S-rich mixture, Na-rich mixture, C/P-rich mixture, and mineral-rich mixture. Consistently, the fraction of biological particles (i.e., P-containing particles) increased when the ship traveled along a strongly biologically active area.

First-year sea ice leads to an increase in dimethyl sulfide-induced particle formation in the Antarctic Peninsula.

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.