Large seasonal and interannual variations of biogenic sulfur compounds in the Arctic atmosphere (Svalbard; 78.9° N, 11.9° E)

Jang, Sehyun; Park, Ki-Tae; Lee, Kitack; Yoon, Young Jun; Kim, Kitae; Chung, Hyun Young; Jang, Eunho; Becagli, Silvia; Lee, Bang Yong; Traversi, Rita; Eleftheriadis, Konstantinos; Krejci, Radovan; Hermansen, Ove

Seasonal to interannual variations in the concentrations of sulfur aerosols (inline-formula< 2.5 inline-formulaµm in diameter; non sea-salt sulfate: NSS-SOinline-formula M5inlinescrollmathml normal 4 normal 2 - 13pt17ptsvg-formulamathimg277c1427ed297c2e5c45f7f988764cfe acp-21-9761-2021-ie00001.svg13pt17ptacp-21-9761-2021-ie00001.png ; anthropogenic sulfate: Anth-SOinline-formula M6inlinescrollmathml normal 4 normal 2 - 13pt17ptsvg-formulamathimg4a53e7d1f00f4334c934356877052515 acp-21-9761-2021-ie00002.svg13pt17ptacp-21-9761-2021-ie00002.png ; biogenic sulfate: Bio-SOinline-formula M7inlinescrollmathml normal 4 normal 2 - 13pt17ptsvg-formulamathimg972fd8e8ae3fad8e22756ca8f92061a6 acp-21-9761-2021-ie00003.svg13pt17ptacp-21-9761-2021-ie00003.png ; methanesulfonic acid: MSA) in the Arctic atmosphere were investigated using measurements of the chemical composition of aerosols collected at Ny-Ålesund, Svalbard (78.9inline-formula N, 11.9inline-formula E) from 2015 to 2019. In all measurement years the concentration of NSS-SOinline-formula M10inlinescrollmathml normal 4 normal 2 - 13pt17ptsvg-formulamathimg6051c44ba131ac206db43e824688e92d acp-21-9761-2021-ie00004.svg13pt17ptacp-21-9761-2021-ie00004.png was highest during the pre-bloom period and rapidly decreased towards summer. During the pre-bloom period we found a strong correlation between NSS-SOinline-formula M11inlinescrollmathml normal 4 normal 2 - 13pt17ptsvg-formulamathimg6181d6711c50a62cc80d469e7dc67eab acp-21-9761-2021-ie00005.svg13pt17ptacp-21-9761-2021-ie00005.png (sum of Anth-SOinline-formula M12inlinescrollmathml normal 4 normal 2 - 13pt17ptsvg-formulamathimg5051a948f61d36bc48409cbb9c9d62b3 acp-21-9761-2021-ie00006.svg13pt17ptacp-21-9761-2021-ie00006.png and Bio-SOinline-formula M13inlinescrollmathml normal 4 normal 2 - 13pt17ptsvg-formulamathimg6ad56f45652d937dfd2349f6d5f05723 acp-21-9761-2021-ie00007.svg13pt17ptacp-21-9761-2021-ie00007.png ) and Anth-SOinline-formula M14inlinescrollmathml normal 4 normal 2 - 13pt17ptsvg-formulamathimg9e5c3b810d685753e2e31321de9aeed4 acp-21-9761-2021-ie00008.svg13pt17ptacp-21-9761-2021-ie00008.png . This was because more than 50 % of the NSS-SOinline-formula M15inlinescrollmathml normal 4 normal 2 - 13pt17ptsvg-formulamathimg9def59c1763723bf85d4c029a1ebd14e acp-21-9761-2021-ie00009.svg13pt17ptacp-21-9761-2021-ie00009.png measured during this period was Anth-SOinline-formula M16inlinescrollmathml normal 4 normal 2 - 13pt17ptsvg-formulamathimg7f75eaded4497f2452ab2c17fc6da474 acp-21-9761-2021-ie00010.svg13pt17ptacp-21-9761-2021-ie00010.png , which originated in northern Europe and was subsequently transported to the Arctic in Arctic haze. Unexpected increases in the concentration of Bio-SOinline-formula M17inlinescrollmathml normal 4 normal 2 - 13pt17ptsvg-formulamathimg31655fb078684da776f2b5262b6b028b acp-21-9761-2021-ie00011.svg13pt17ptacp-21-9761-2021-ie00011.png aerosols (an oxidation product of dimethylsulfide: DMS) were occasionally found during the pre-bloom period. These probably originated in regions to the south (the North Atlantic Ocean and the Norwegian Sea) rather than in ocean areas in the proximity of Ny-Ålesund. Another oxidation product of DMS is MSA, and the ratio of MSA to Bio-SOinline-formula M18inlinescrollmathml normal 4 normal 2 - 13pt17ptsvg-formulamathimgcc76bdecf8cb88b8edd7164534c60e80 acp-21-9761-2021-ie00012.svg13pt17ptacp-21-9761-2021-ie00012.png is extensively used to estimate the total amount of DMS-derived aerosol particles in remote marine environments. The concentration of MSA during the pre-bloom period remained low, primarily because of the greater loss of MSA relative to Bio-SOinline-formula M19inlinescrollmathml normal 4 normal 2 - 13pt17ptsvg-formulamathimg49798bc14746e7788afe38c7f4bc425f acp-21-9761-2021-ie00013.svg13pt17ptacp-21-9761-2021-ie00013.png and the suppression of condensation of gaseous MSA onto particles already present in air masses being transported northwards from distant ocean source regions (existing particles). In addition, the low light intensity during the pre-bloom period resulted in a low concentration of photochemically activated oxidant species including OH radicals and BrO; these conditions favored the oxidation pathway of DMS to Bio-SOinline-formula M20inlinescrollmathml normal 4 normal 2 - 13pt17ptsvg-formulamathimg9b4424a385540adc94d244c67eeed79b acp-21-9761-2021-ie00014.svg13pt17ptacp-21-9761-2021-ie00014.png rather than to MSA, which acted to lower the MSA concentration at Ny-Ålesund. The concentration of MSA peaked in May or June and was positively correlated with phytoplankton biomass in the Greenland and Barents seas around Svalbard. As a result, the mean ratio of MSA to the DMS-derived aerosols was low (0.09 inline-formula± 0.07) in the pre-bloom period but high (0.32 inline-formula± 0.15) in the bloom and post-bloom periods. There was large interannual variability in the ratio of MSA to Bio-SOinline-formula M23inlinescrollmathml normal 4 normal 2 - 13pt17ptsvg-formulamathimg0c8dda110a7ac5e3eb0d9cbeda0d9b58 acp-21-9761-2021-ie00015.svg13pt17ptacp-21-9761-2021-ie00015.png (i.e., 0.24 inline-formula± 0.11 in 2017, 0.40 inline-formula± 0.14 in 2018, and 0.36 inline-formula± 0.14 in 2019) during thepage9762 bloom and post-bloom periods. This was probably associated with changes in the chemical properties of existing particles, biological activities surrounding the observation site, and air mass transport patterns. Our results indicate that MSA is not a conservative tracer for predicting DMS-derived particles, and the contribution of MSA to the growth of newly formed particles may be much larger during the bloom and post-bloom periods than during the pre-bloom period.

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Jang, Sehyun / Park, Ki-Tae / Lee, Kitack / et al: Large seasonal and interannual variations of biogenic sulfur compounds in the Arctic atmosphere (Svalbard; 78.9° N, 11.9° E). 2021. Copernicus Publications.

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