Sea spray aerosol (SSA) can have complex carbon speciation that is affected by biological conditions in the seawater from which it originates. Biologically derived molecules can also interact with other longer-lived organic and inorganic carbon species in the sea surface microlayer and in the process of bubble bursting. An isolated wave channel facility was used to generate sea spray aerosol during a 1 month mesocosm study. Two consecutive phytoplankton blooms occurred, and sea spray aerosol was sampled throughout. Scanning transmission X-ray microscopy coupled with near-edge X-ray absorption fine structure spectroscopy (STXM-NEXAFS) was used to determine spatially resolved carbon speciation within individual particles from 0.18 to 3.2 μm. During phytoplankton blooms, coarse-mode particles exhibited an increased abundance of carboxylic acid-rich needlelike structures. The extent of organic enrichment in fine-mode particles correlates with the occurrence of aliphatic-rich organic species, as detected by an intense C 1s → σ(C–H)* excitation. These aliphatic-rich species had a strong association with graphitic carbon, as detected by a C 1s → σ* exciton excitation. This enrichment was unique to particles collected in the aerodynamic size range 0.18–0.32 μm and corresponded with the decrease in hygroscopicity. Aliphatic organics can significantly suppress the particle hygroscopicity when they replace salt, thus influencing the effect of sea spray aerosol on light scattering and cloud formation. These results suggest that graphitic carbon is concentrated in the sea surface microlayer during phytoplankton blooms and released through wave action. These results may have implications for radiative transfer and carbon cycling in the ocean–atmosphere system.

中文翻译：

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生物对海水喷雾气溶胶碳形态和形态的影响

海水喷雾气溶胶（SSA）可能具有复杂的碳形态，受其起源的海水中生物条件的影响。生物衍生的分子还可以在海面微层中以及在气泡破裂过程中与其他寿命更长的有机和无机碳物种发生相互作用。在为期1个月的中观研究中，使用了隔离的波浪通道设施产生海雾气溶胶。发生了两次连续的浮游植物水华，并在整个过程中取样了海喷雾气溶胶。扫描透射X射线显微镜和近边缘X射线吸收精细结构光谱（STXM-NEXAFS）用于确定0.18至3.2μm单个颗粒内的空间分辨碳形态。在浮游植物开花期间，粗模式颗粒显示出丰富的富含羧酸的针状结构。细模式颗粒中有机物富集的程度与富含脂肪族有机物的发生有关，如通过强烈的C 1s→σ（C–H）*激发所检测到的。通过C 1s→σ*激子激发可以发现，这些富含脂肪族的物质与石墨碳有很强​​的联系。这种富集是在空气动力学尺寸范围为0.18–0.32μm范围内收集到的颗粒所独有的，并且与吸湿性的降低相对应。脂肪族有机物代替盐时，可以显着抑制颗粒的吸湿性，从而影响海上喷雾气溶胶对光散射和云团形成的影响。这些结果表明，在浮游植物开花期间，石墨碳集中在海表微层中，并通过波动作用释放出来。这些结果可能会对海洋-大气系统中的辐射传递和碳循环产生影响。