Abstract
Abstract. The tropical and subtropical Indian Ocean (IO) is expected to be a significant source of water-soluble organic aerosols (WSOAs), which are important factors relevant to cloud formation of aerosol particles. Current atmospheric numerical models significantly underestimate the budget of organic aerosols and their precursors, especially over tropical oceans. This is primarily due to poor knowledge of sources and the paucity of observations of these parameters considering spatial and temporal variation over the tropical open ocean. To evaluate the contribution of sources to WSOA as well as their formation processes, submicrometer aerosol sampling was conducted at the high-altitude Maïdo observatory (21.1∘ S, 55.4∘ E; 2160 m a.s.l.), located on the remote island of La Réunion in the southwest IO. The aerosol samples were continuously collected during local daytime and nighttime, which corresponded to the ambient conditions of the marine boundary layer (MBL) and free troposphere (FT), respectively, from 15 March to 24 May 2018. Chemical analysis showed that organic matter was the dominant component of submicrometer water-soluble aerosol (∼ 45 ± 17 %) during the wet season (15 March–23 April). On the other hand, sulfate dominated (∼ 77 ± 17 %) during the dry season (24 April–24 May), most of which was attributable to the effect of volcanic eruption. Measurements of the stable carbon isotope ratio of water-soluble organic carbon (WSOC) suggested that marine sources contributed significantly to the observed WSOC mass in both the MBL and the FT in the wet season, whereas a mixture of marine and terrestrial sources contributed to WSOC in the dry season. The distinct seasonal changes in the dominant source of WSOC were also supported by Lagrangian trajectory analysis. Positive matrix factorization analysis suggested that marine secondary organic aerosol (OA) dominantly contributed to the observed WSOC mass (∼ 70 %) during the wet season, whereas mixtures of marine and terrestrial sources contributed during the dry season in both MBL and FT. Overall, this study demonstrates that the effect of marine secondary sources is likely important up to the FT in the wet season, which may affect cloud formation as well as direct radiative forcing over oceanic regions.
Highlights
The ocean is a major source of submicrometer aerosols, which play an important role in the atmospheric radiative budget because they determine the number of cloud condensation nuclei (CCN) and ice nuclei (IN)
The wet season was defined as the first half of the sampling period, whereas the latter half was defined as the dry season reflecting the significant difference in the water vapor mixing ratios between wet (8.7 ± 2.6 g kg−1) and dry seasons (6.4 ± 1.4 g kg−1), where the confidence interval of 95 % for the difference is higher than zero
The results presented in this study confirm that the observatory was located in the marine boundary layer (MBL) during daytime, whereas it was in the free troposphere (FT) at night
Summary
The ocean is a major source of submicrometer aerosols, which play an important role in the atmospheric radiative budget because they determine the number of cloud condensation nuclei (CCN) and ice nuclei (IN). Marine-derived submicrometer organic aerosols (OAs) can affect the marine aerosol optical depth (AOD) as well as CCN and IN concentrations. These are important over remote oceans, as these areas experience minimal influence from anthropogenic emissions originating from terrestrial sources. Sea-to-air emissions of volatile organic compounds (VOCs) produced by marine microbial activity have the potential to form secondary OAs. there is still a large uncertainty in the potential sources and formation processes of OA in the marine atmosphere, leading to uncertainty in determining their climate impact
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