Organic composition of three different size ranges of aerosol particles over the Southern Ocean
Organic composition of three different size ranges of aerosol particles over the Southern Ocean
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南大洋上空三种不同尺寸范围的气溶胶颗粒的有机成分
DOI：
10.1080/02786826.2020.1845296
复制
发表时间：
2021
影响因子：
5.2
通讯作者：
DeMott, P. J.
中科院分区：
文献类型：
--
作者：
Saliba, G.;Sanchez, K. J.;Russell, L. M.;Twohy, C. H.;Roberts, G. C.;Lewis, S.;Dedrick, J.;McCluskey, C. S.;Moore, K.;DeMott, P. J.
很少有测量存在的组成和云凝结核（CCN）的有机质量（OM）在不同大小的粒子在南大洋。在南大洋云、辐射、气溶胶输送试验研究期间有机成分、气溶胶数量和质量大小分布以及CCN谱的空中和船上测量（SOCRATES）提供了三种不同尺寸范围的有机贡献的比较：（1）通过扫描透射X射线显微镜（STXM）和近边X射线吸收精细结构（NEXAFS）对直径为0.25-1.75 µm的颗粒进行分析，（2）通过扫描透射电子显微镜和能量色散X射线光谱法（STEM-EDS）对直径为0.1-0.5和0.5-1µm的颗粒进行分析，以及（3）间接通过比较CCN光谱与直径<0.15 µm的颗粒的粒度分布进行分析。来自STXM-NEXAFS显微镜的有机官能团表明，大多数直径在0.25和1.75 µm之间的颗粒具有可检测的有机成分，与与海喷雾颗粒相关的海洋有机特征一致，这也适用于通过浸没冷冻<−27 °C取样的冰成核颗粒。对96个NEXAFS光谱进行聚类，得到5种不同类型的与海雾相关的有机混合物（4种含盐海雾颗粒类型和1种富含有机物的颗粒类型，不含盐核），占颗粒的76%，其中2种为原生颗粒，3种为可能来自次生来源的酸性基团。STEM分析表明，直径为0.1-0.5微米的颗粒主要是硫酸盐，直径为0.5-1微米的颗粒主要是钠基海雾。大多数直径>0.1 µm的颗粒的吸湿性与钠基海雾和硫酸盐颗粒一致，从而在STEM和CCN测量之间提供闭合。直径<0.15 µm的颗粒的kappa值为0.2-0.5，表明在这些尺寸下大量存在OM。通过比较粒径分布和过饱和度光谱估计的有机组分分数在<10%至70%之间变化，颗粒直径<0.15 µm。该结果显示了在SO典型过饱和下，直径<0.15 µm的颗粒的有机组成对CCN浓度的影响。这种可变的OM分数占小于0.15 µm直径的颗粒的质量浓度<0.1 µg/m3，但可能在云过饱和度大于0.3%时发挥作用。
Very few measurements exist of the composition and contribution to cloud condensation nuclei (CCN) of organic mass (OM) at different sizes for particles over the Southern Ocean. Airborne and shipboard measurements of organic composition, aerosol number and mass size distributions, and CCN spectra during the Southern Ocean Clouds, Radiation, Aerosol Transport Experimental Study (SOCRATES) provide a comparison of organic contributions at three different size ranges: (1) by scanning transmission X-ray microscope (STXM) with near edge X-ray absorption fine structure (NEXAFS) for particles 0.25–1.75 µm diameter, (2) by scanning transmission electron microscopy with energy dispersive X-ray spectroscopy (STEM-EDS) for particles 0.1–0.5 and 0.5–1µm diameter, and (3) indirectly by comparing CCN spectra to particle size distributions for particles <0.15 µm diameter. Organic functional groups from STXM-NEXAFS microscopy indicate that the majority of particles between 0.25 and 1.75 µm diameter with detectable organic components were consistent with marine organic signatures associated with sea spray particles, which was also true for ice nucleating particles sampled by immersion freezing <−27 °C. Clustering of the 96 NEXAFS spectra resulted in 5 distinct types of sea spray related organic mixtures (four salt-containing sea spray particle types and one organic-rich particle type without a salt core) that accounted for 76% of the particles, including two that appear primary and three that include acid groups that are likely from secondary sources. STEM analysis indicates that particles 0.1–0.5 µm diameter were mostly sulfate and particles 0.5–1 µm diameter were mostly sodium-based sea spray. The hygroscopicity of most particles >0.1 µm diameter were consistent with sodium-based sea spray and sulfate particles, providing closure between STEM and CCN measurements. Particles <0.15 µm diameter had kappa values of 0.2–0.5, indicating the substantial presence of OM at these sizes. The organic component fraction estimated from comparing the size distribution and supersaturation spectra varied from <10% to 70% for particles <0.15 µm diameter. This result shows the impact of the organic composition of particles <0.15 µm diameter on CCN concentrations at typical supersaturations for the SO. This variable OM fraction accounted for <0.1 µg/m3mass concentrations of particles smaller than 0.15 µm diameter but may play a role at cloud supersaturations greater than 0.3%.Copyright © 2020 American Association for Aerosol Research
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