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Resolving the mechanisms of hygroscopic growth and cloud condensation nuclei activity for organic particulate matter.

ABSTRACT: 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.

SUBMITTER: Liu P

PROVIDER: S-EPMC6172236 | biostudies-literature | 2018 Oct

REPOSITORIES: biostudies-literature

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Resolving the mechanisms of hygroscopic growth and cloud condensation nuclei activity for organic particulate matter.

Liu Pengfei P Song Mijung M Zhao Tianning T Gunthe Sachin S SS Ham Suhan S He Yipeng Y Qin Yi Ming YM Gong Zhaoheng Z Amorim Juliana C JC Bertram Allan K AK Martin Scot T ST

Nature communications 20181004 1

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 representativ ...[more]

PMID: 30287821

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Project description:Coastal southeast Florida experiences a wide range of aerosol conditions, including African dust, biomass burning (BB) aerosols, as well as sea salt and other locally-emitted aerosols. These aerosols are important sources of cloud condensation nuclei (CCN), which play an essential role in governing cloud radiative properties. As marine environments dominate the surface of Earth, CCN characteristics in coastal southeast Florida have broad implications for other regions with the added feature that this site is perturbed by both natural and anthropogenic emissions. This study investigates the influence of different air mass types on CCN concentrations at 0.2% (CCN0.2%) and 1.0% (CCN1.0%) supersaturation (SS) based on ground site measurements during selected months in 2013, 2017, and 2018. Average CCN0.2% and CCN1.0% concentrations were 373 ± 200 cm-3 and 584 ± 323 cm-3, respectively, for four selected days with minimal presence of African dust and BB (i.e., background days). CCN concentrations were not elevated on the four days with highest influence of African dust (289 ± 104 cm-3 [0.2% SS] and 591 ± 302 cm-3 [1.0% SS]), consistent with high dust mass concentrations comprised of coarse particles that are few in number. In contrast, CCN concentrations were substantially enhanced on the five days with the greatest impact from BB (1408 ± 976 cm-3 [0.2% SS] and 3337 ± 1252 cm-3 [1.0% SS]). Ratios of CCN0.2%:CCN1.0% were used to compare the hygroscopicity of the aerosols associated with African dust, BB, and background days. Average ratios were similar for days impacted by African dust and BB (0.54 ± 0.17 and 0.55 ± 0.17, respectively). A 29% higher average ratio was observed on background days (0.71 ± 0.14), owing in part to a strong presence of sea salt and reduced presence of more hydrophobic species such as those of a carbonaceous or mineral-dust nature. Finally, periods of heavy rainfall were shown to effectively decrease both CCN0.2% and CCN1.0% concentrations. However, the rate varied at which such concentrations increased after the rain. This work contributes knowledge on the nucleating ability of African dust and BB in a marine environment after varying periods of atmospheric transport (days to weeks). The results can be used to understand the hygroscopicity of these air mass types, predict how they may influence cloud properties, and provide a valuable model constraint when predicting CCN concentrations in comparable situations.

Dataset Information

Resolving the mechanisms of hygroscopic growth and cloud condensation nuclei activity for organic particulate matter.

Publications

Resolving the mechanisms of hygroscopic growth and cloud condensation nuclei activity for organic particulate matter.

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