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Aircraft measurements of aerosol and trace gas chemistry in the eastern North Atlantic

机译：北大西洋东部气溶胶和痕量气体化学的飞机测量

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The Aerosol and Cloud Experiment in the Eastern North Atlantic?(ACE-ENA) investigated properties of aerosols and subtropical marine boundary layer?(MBL) clouds. Low subtropical marine clouds can have a large effect on Earth's radiative budget, but they are poorly represented in global climate models. In order to understand their radiative effects, it is imperative to understand the composition and sources of the MBL cloud condensation nuclei?(CCN). The campaign consisted of two intensive operation periods?(IOPs) (June–July?2017 and January–February?2018) during which an instrumented G-1?aircraft was deployed from Lajes Field on Terceira Island in the Azores, Portugal. The G-1?conducted research flights in the vicinity of the Atmospheric Radiation Measurement?(ARM) Eastern North Atlantic?(ENA) atmospheric observatory on Graciosa Island. An Aerodyne high-resolution time-of-flight aerosol mass spectrometer?(HR-ToF-AMS) and Ionicon proton-transfer-reaction mass spectrometer?(PTR-MS) were deployed aboard the aircraft, characterizing chemistry of non-refractory aerosol and trace gases, respectively. The eastern North Atlantic region was found to be very clean, with an average non-refractory submicrometer aerosol mass loading of 0.6? μ g?m ?3 in the summer and 0.1? μ g?m ?3 in the winter, measured by the AMS. Average concentrations of the trace reactive gases methanol and acetone were 1–2?ppb; benzene, toluene and isoprene were even lower, 1 ?ppb. Mass fractions of sulfate, organics, ammonium and nitrate in the boundary layer were 69?%, 23?%, 7?% and 1?% and remained largely similar between seasons. The aerosol chemical composition was dominated by sulfate and highly processed organics. Particulate methanesulfonic acid?(MSA), a well-known secondary biogenic marine species, was detected, with an average boundary layer concentration of 0.021? μ g?m ?3 , along with its gas-phase precursor, dimethyl sulfide?(DMS). MSA accounted for no more than 3?% of the submicron, non-refractory aerosol in the boundary layer. Examination of vertical profiles of aerosol and gas chemistry during ACE-ENA reveals an interplay of local marine emissions and long-range-transported aged aerosol. A case of transport of biomass burning emissions from North American fires has been identified using back-trajectory analysis. In the summer, the non-refractory portion of the background CCN budget was heavily influenced by aerosol associated with ocean productivity, in particular sulfate formed from DMS oxidation. Episodic transport from the continents, particularly of biomass burning aerosol, periodically increased CCN concentrations in the free troposphere. In the winter, with ocean productivity lower, CCN concentrations were overall much lower and dominated by remote transport. These results show that anthropogenic emissions perturb CCN concentrations in remote regions that are sensitive to changes in CCN number and illustrate that accurate predictions of both transport and regional aerosol formation from the oceans are critical to accurately modeling clouds in these regions.
机译：东北大西洋的气溶胶和云实验？（ACE-ena）调查了气溶胶和亚热带船舶边界层的性质？（MBL）云。低亚热带的海洋云可以对地球辐射预算产生很大影响，但它们在全球气候模型中差不多。为了了解他们的辐射效果，必须了解MBL云凝结核的组成和来源？（CCN）。该活动由两个密集的运营期组成？（IOPS）（2017年6月至2017年和1月 - 2月？2018），在此期间从葡萄牙亚速尔斯·塔尔斯的Ticeira Island上部署了一个仪器的G-1？飞机。 G-1？在大气辐射测量附近进行了研究航班？（ARM）东部大西洋（ENA）Graciosa Island的大气天文台。 Aerodyne高分辨率飞行时间气溶胶质谱仪？（HR-TOF-AMS）和离子质子转移反应质谱仪？（PTR-MS）被部署在飞机上，表征了非难治气溶胶的化学和分别痕量气体。发现东北大西洋地区非常干净，平均非难治性亚微米器气溶胶质量荷载0.6？ μg？m？3夏天和0.1？ μg？m？3在冬天，由AMS测量。痕量反应气体甲醇和丙酮的平均浓度为1-2μl; ppb;苯，甲苯和异戊二烯甚至更低，＆ 1？ppb。边界层中硫酸盐，有机物，铵和硝酸盐的质量分数为69〜％，23μm，7μ％，7μl％，在季节之间存在很大类似。气溶胶化学组合物通过硫酸盐和高加工的有机物占主导地位。颗粒状甲烷磺酸α（MSA），检测着众所周知的二次生物海洋物种，平均边界层浓度为0.021？ μg≤m≤3，以及其气相前体，二甲基硫醚？（DMS）。 MSA占亚微米，非难治性气溶胶中的3个超过3？％。在ACE-ENA期间检查气溶胶和天然气化学垂直曲线揭示了当地海洋排放和远程运输的昔日气溶胶的相互作用。使用反轨道分析确定了北美火灾燃烧排放的生物质排放的情况。在夏季，背景CCN预算的非难熔部分受到与海洋生产力相关的气溶胶的严重影响，特别是由DMS氧化形成的硫酸盐。来自大陆的焦点运输，特别是生物质燃烧气溶胶，周期性地增加了自由对流层中的CCN浓度。在冬季，随着海洋生产力降低，CCN浓度总体整体下降得多，并以远程运输为主。这些结果表明，对CCN数变化敏感的偏远地区的人为排放扰动CCN浓度，并说明，从海洋中的运输和区域气溶胶形成的准确预测对于准确地建模这些地区的云是至关重要的。

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