Resolving the mechanisms of hygroscopic growth and cloud condensation nuclei activity for organic particulate matter.
Resolving the mechanisms of hygroscopic growth and cloud condensation nuclei activity for organic particulate matter.
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DOI：
10.1038/s41467-018-06622-2
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发表时间：
2018-10-04
影响因子：
16.6
通讯作者：
Martin ST
中科院分区：
文献类型：
--
作者：
Liu P;Song M;Zhao T;Gunthe SS;Ham S;He Y;Qin YM;Gong Z;Amorim JC;Bertram AK;Martin ST
吸湿增长和云凝结核激活是精确模拟有机颗粒物气候影响的关键过程。然而，这些过程的微观物理机制仍然没有解决。在这里，我们报告了复杂的热力学行为，包括与湿度有关的吸湿性，与直径有关的云凝结核活动，以及实验室中代表相似大气有机颗粒物的生物来源次生有机物质的液-液相分离。这些行为可以用水与疏水性和亲水性有机成分的非理想混合来解释。非理想驱动的液液相分离进一步增强了水的吸收，并在高相对湿度下导致表面张力降低，从而降低了云凝结核激活的势垒。相比之下，代表人为来源的次生有机物质并不表现出复杂的热力学行为。综合结果突出了在地球气候系统模型中对吸湿性和云凝结核活动的详细热力学表示的重要性。有机颗粒物和水蒸气之间的相互作用影响气候预测，但这些相互作用的机制仍未解决。在这里，作者提出了一个相分离机制，它协调了观测到的吸湿性和云凝结核活动。
Hygroscopic growth and cloud condensation nuclei activation are key processes for accurately modeling the climate impacts of organic particulate matter. Nevertheless, the microphysical mechanisms of these processes remain unresolved. Here we report complex thermodynamic behaviors, including humidity-dependent hygroscopicity, diameter-dependent cloud condensation nuclei activity, and liquid–liquid phase separation in the laboratory for biogenically derived secondary organic material representative of similar atmospheric organic particulate matter. These behaviors can be explained by the non-ideal mixing of water with hydrophobic and hydrophilic organic components. The non-ideality-driven liquid–liquid phase separation further enhances water uptake and induces lowered surface tension at high relative humidity, which result in a lower barrier to cloud condensation nuclei activation. By comparison, secondary organic material representing anthropogenic sources does not exhibit complex thermodynamic behavior. The combined results highlight the importance of detailed thermodynamic representations of the hygroscopicity and cloud condensation nuclei activity in models of the Earth’s climate system. The interactions between organic particulate matter and water vapour affect climate predictions, yet the mechanisms of these interactions remain unresolved. Here, the authors propose a phase separation mechanism that reconciles the observed hygroscopicity and cloud condensation nuclei activity.
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