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Physicochemical Mixing State of Sea Spray Aerosols: Morphologies Exhibit Size Dependence
ACS Earth and Space Chemistry ( IF 2.9 ) Pub Date : 2020-08-04 , DOI: 10.1021/acsearthspacechem.0c00153 Hansol D. Lee 1 , Samantha Wigley 1 , Christopher Lee 2 , Victor W. Or 3 , Elias S. Hasenecz 1 , Elizabeth A. Stone 1 , Vicki H. Grassian 2, 3 , Kimberly A. Prather 2, 3, 4 , Alexei V. Tivanski 1
ACS Earth and Space Chemistry ( IF 2.9 ) Pub Date : 2020-08-04 , DOI: 10.1021/acsearthspacechem.0c00153 Hansol D. Lee 1 , Samantha Wigley 1 , Christopher Lee 2 , Victor W. Or 3 , Elias S. Hasenecz 1 , Elizabeth A. Stone 1 , Vicki H. Grassian 2, 3 , Kimberly A. Prather 2, 3, 4 , Alexei V. Tivanski 1
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Sea spray aerosols (SSA) play an important role in radiative forcing by directly scattering solar radiation and indirectly by acting as cloud condensation or ice nuclei. These climate-relevant aerosol processes strongly depend on the mixing state and morphology of the individual aerosol. In this work, the distribution of different morphologies within nascent SSA as a function of particle size is investigated. SSA generated from wave breaking of natural seawater were collected for offline analysis using complementary scanning electron microscopy (SEM), thermal optical analysis, and atomic force microscopy-based photothermal infrared (AFM-PTIR) spectroscopy methods. SEM data revealed six key morphologies of SSA—prism-like, core–shell, rounded, rod-inclusion, aggregate, and rod. Of these, prism-like, core–shell, and rounded morphologies accounted for more than 99% of the entire SSA population and exhibited size-dependent trends. Thermal optical analysis data revealed a significant increase in the organic mass fraction of SSA with decreasing particle size. Concurrently, the SEM data showed a significant decrease in the relative abundance of prism-like morphology and corresponding increase of rounded and core–shell morphologies. AFM-PTIR spectroscopy showed that the SSA prism-like morphology is largely inorganic in nature, whereas the shell of the core–shell and rounded morphologies are predominantly organic. The study demonstrates that, instead of a single “representative” SSA morphology, the physicochemical mixing state of SSA is dynamic with respect to particle size. This should be taken into account to accurately predict the magnitude of the radiative forcing of SSA.
中文翻译：
海喷雾气溶胶的物理化学混合状态：形态表现出尺寸依赖性
海洋喷雾气溶胶（SSA）通过直接散射太阳辐射并间接充当云凝结或冰核间接在辐射强迫中发挥重要作用。这些与气候有关的气溶胶过程在很大程度上取决于单个气溶胶的混合状态和形态。在这项工作中，研究了新生SSA中不同形态的分布与粒径的关系。收集了从天然海水的波浪破碎产生的SSA，以使用互补扫描电子显微镜（SEM），热光学分析和基于原子力显微镜的光热红外（AFM-PTIR）光谱学方法进行离线分析。SEM数据显示了SSA的六种主要形态-棱镜状，核-壳状，圆形，棒状夹杂物，骨料和棒状。其中，棱柱状的核壳，圆形形态占整个SSA人口的99％以上，并且呈现出大小依赖的趋势。热光学分析数据显示，随着粒度的减小，SSA的有机质量分数显着增加。同时，SEM数据显示，棱柱状形态的相对丰度显着下降，而圆形和核-壳形态的相对丰度相应增加。AFM-PTIR光谱显示，SSA棱柱状形态在很大程度上是无机的，而核-壳和圆形形态的壳则主要是有机的。该研究表明，SSA的物理化学混合状态不是唯一的“代表性” SSA形态，而是相对于粒径而言是动态的。
更新日期：2020-09-18
中文翻译：
海喷雾气溶胶的物理化学混合状态：形态表现出尺寸依赖性
海洋喷雾气溶胶（SSA）通过直接散射太阳辐射并间接充当云凝结或冰核间接在辐射强迫中发挥重要作用。这些与气候有关的气溶胶过程在很大程度上取决于单个气溶胶的混合状态和形态。在这项工作中，研究了新生SSA中不同形态的分布与粒径的关系。收集了从天然海水的波浪破碎产生的SSA，以使用互补扫描电子显微镜（SEM），热光学分析和基于原子力显微镜的光热红外（AFM-PTIR）光谱学方法进行离线分析。SEM数据显示了SSA的六种主要形态-棱镜状，核-壳状，圆形，棒状夹杂物，骨料和棒状。其中，棱柱状的核壳，圆形形态占整个SSA人口的99％以上，并且呈现出大小依赖的趋势。热光学分析数据显示，随着粒度的减小，SSA的有机质量分数显着增加。同时，SEM数据显示，棱柱状形态的相对丰度显着下降，而圆形和核-壳形态的相对丰度相应增加。AFM-PTIR光谱显示，SSA棱柱状形态在很大程度上是无机的，而核-壳和圆形形态的壳则主要是有机的。该研究表明，SSA的物理化学混合状态不是唯一的“代表性” SSA形态，而是相对于粒径而言是动态的。
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