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Low-Volatility Vapors and New Particle Formation Over the Southern Ocean During the Antarctic Circumnavigation Expedition

机译:南极环球航行探险期间南大洋上空的低挥发性蒸气和新颗粒形成

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摘要

During summer, the Southern Ocean is largely unaffected by anthropogenic emissions, which makes this region an ideal place to investigate marine natural aerosol sources and processes. A better understanding of natural aerosol is key to constrain the preindustrial aerosol state and reduce the aerosol radiative forcing uncertainty in global climate models. We report the concentrations of gaseous sulfuric acid, iodic acid, and methanesulfonic acid (MSA) together with a characterization of new particle formation (NPF) events over a large stretch of the Southern Ocean. Measurements were conducted on board the Russian icebreaker Akademik Tryoshnikov from January to March 2017. Iodic acid is characterized by a particular diurnal cycle with reduced concentration around noon, suggesting a lower formation yield when solar irradiance is higher. Gaseous MSA does not have a diurnal cycle and measured concentrations in gas and condensed phase are compatible with this species being primarily produced via heterogeneous oxidation of dimethyl sulfide and subsequent partitioning into the gas phase. We also found that NPF in the boundary layer is mainly driven by sulfuric acid but it occurred very rarely over the vast geographical area probed and did not contribute to the cloud condensation nuclei budget in a directly observable manner. Despite the near absence of NPF events in the boundary layer, Aitken mode particles were frequently measured, supporting the hypothesis of a free tropospheric source. Iodic acid and MSA were not found to participate in nucleation, however, MSA may contribute to aerosol growth via heterogeneous formation in the aqueous phase.
机译:在夏季,南大洋基本上不受人为排放的影响,这使得该地区成为调查海洋天然气溶胶来源和过程的理想场所。更好地了解天然气溶胶是约束工业化前气溶胶状态和降低全球气候模式中气溶胶辐射强迫不确定性的关键。我们报告了气态硫酸、碘酸和甲磺酸 (MSA) 的浓度,以及南大洋大片新颗粒形成 (NPF) 事件的特征。测量是在1月至3月2017的俄罗斯破冰船Akademik Tryoshnikov上进行的。碘酸的特征是特定的昼夜循环,中午前后浓度降低,表明当太阳辐照度较高时,地层产率较低。气态MSA没有昼夜循环,气体和冷凝相中测得的浓度与该物质相容,主要通过二甲基硫醚的非均相氧化和随后的分配到气相中产生。我们还发现,边界层的NPF主要由硫酸驱动,但在探测到的广阔地理区域内很少发生,并且没有直接观测到对云凝结核预算的贡献。尽管边界层中几乎没有NPF事件,但经常测量Aitken模式粒子,支持自由对流层源的假设。未发现碘酸和MSA参与成核,但是,MSA可能通过水相中的非均相形成促进气溶胶生长。

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