It is critical to understand how variations in chemical composition in surface seawater (SSW) affect the chemistry of marine atmospheric aerosols. We investigated the sea-to-air transfer of dissolved organic carbon (DOC) via cruise measurements of both ambient aerosols and SSW in the Oyashio and its coastal regions, the western subarctic Pacific during early spring. Sea spray aerosols (SSAs) were selected based on the stable carbon isotope ratio of water-soluble organic carbon (WSOC) (δ13CWSOC) and concentrations of glucose as a molecular tracer in marine aerosols together with local surface wind speed data. For both SSA and SSW samples, excitation-emission matrices were obtained to examine the transfer of fluorescent organic material. We found that the ratios of fluorescence intensity of humic-like and protein-like substances in the submicrometer SSAs were significantly larger than those in the bulk SSW (~63%). This ratio was also larger for the supermicrometer SSAs than for the SSW. The results suggest significant decomposition of protein-like DOC on a timescale of <12–24 h and/or preferential production of humic-like substances in the atmospheric aerosols regardless of the particle size. This study provides unique insights into the complex transfer of DOC from the ocean surface to the atmosphere.
The size‐resolved distributions of hygroscopic growth factor g and the ratios of cloud condensation nuclei (CCN) to condensation nuclei of atmospheric aerosols were investigated in Nagoya, Japan. The average of the distributions of g at 85% relative humidity was bimodal. The size‐resolved mean κ derived from g showed an increasing trend with diameter: 0.17–0.33 at 24–359 nm. The κ values calculated from CCN activation curves were 37% higher than those derived from g. Only 9% of the 37% difference is explained by the difference in the κ of inorganics under subsaturated and supersaturated conditions, suggesting a contribution of organics to the remaining 28% difference. The size‐averaged κ of organics (κorg) was calculated as 0.14 and 0.19 by two different methods. The number fractions of CCN predicted from the hygroscopicity data over the range of 24–359 nm are loosely consistent with those observed if the size‐ and time‐averaged g is applied to all particles (differences: −30% to +10%). This consistency improves if size‐ and time‐resolved g and g distribution are used (differences: −19% to −3%). Whereas the number fractions of CCN predicted from the composition data are greatly underestimated if organics are assumed to be insoluble (differences: −64% to −45%), they are more consistent if κorg of 0.14 or 0.19 is applied (differences: −10% to +14%). The results demonstrate the importance of the dependence of the g of particles on time and particle size and the hygroscopicity of organics for CCN number concentrations in the urban atmosphere.
The formation of biogenic secondary organic aerosols (BSOAs) in forest environments is potentially important to cloud formation via changes of the cloud condensation nuclei (CCN) activity of aerosols. In this study, the CCN activation of submicrometer aerosols and their chemical compositions and size distributions were measured at a midlatitude forest site in Japan during the summer of 2014 to assess the hygroscopicity of the organic aerosols and their contributions to the local CCN concentrations. The mean number concentrations of the condensation nuclei and CCN at supersaturation (SS) conditions of 0.11–0.80% were 1,238 and 166–740 cm−3, respectively. Organic aerosols and sulfate dominated the submicrometer aerosol mass concentrations. The particle hygroscopicity increased with increases in particle diameters. The hygroscopicity parameter for the organics, κorg, was positively correlated with the atomic O to C ratio. The product of κorg and the volume fraction of OA was 0.12, accounting for 38% of the water uptake by aerosol particles. The hygroscopicity parameter of the locally formed fresh BSOA was estimated to be 0.09. The contribution of OA to the CCN number concentration, which was assessed by subtracting the CCN concentration of the hypothetical inorganic aerosols from that of the ambient aerosols, was 50–182 cm−3 for the SS range of 0.11–0.80%. The increase of the CCN number concentrations per 1‐μg/m3 increase of the BSOA was 23–299 cm−3 at 0.11–0.80% SS. The contribution of the BSOA to the CCN number concentration can be enhanced by new particle formation.
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