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DOI	10.5194/acp-22-4149-2022
	On the evolution of sub- and super-saturated water uptake of secondary oraanic aerosol in chamber experiments from mixed precursors
	Wang, Yu; Voliotis, Aristeidis; Hu, Dawei; Shao, Yunqi; Du, Mao; Chen, Ying; Kleinheins, Judith; Marcolli, Claudia; Alfarra, M. Rami; McFiggans, Gordon
发表日期	2022
ISSN	1680-7316
EISSN	1680-7324
起始页码	4149
结束页码	4166
卷号	22 期号:6 页码:18
英文摘要	To better understand the chemical controls of sub- and super-saturated aerosol water uptake, we designed and conducted a series of chamber experiments to investigate the evolution of secondary organic aerosol (SOA) particle physicochemical properties during photo-oxidation of single and mixed biogenic (alpha-pinene, isoprene) and anthropogenic (o-cresol) volatile organic compounds (VOCs) in the presence of ammonium sulfate seeds. During the 6 h experiments, the cloud condensation nuclei (CCN) activity at super-saturation of water (0.1 %-0.5 %), hygroscopic growth factor at 90 % relative humidity (RH), and non-refractory PM) chemical composition were recorded concurrently. Attempts to use the hygroscopicity parameter kappa to reconcile water uptake ability below and above water saturation from various VOC precursor systems were made, aiming to predict the CCN activity from the sub-saturated hygroscopicity. The thermodynamic model AIOMFAC (aerosol inorganic-organic mixtures functional groups activity coefficients) was used to simulate kappa values of model compound mixtures to compare with the observation and to isolate the controlling factors of water uptake at different RHs. The sub- and super-saturated water uptake (in terms of both kappa(HTDMA) and kappa(CC)(N)) were mainly controlled by the SOA mass fraction, which depended on the SOA production rate of the precursors, and the SOA composition played a second-order role. For the reconciliation of kappa(HTDMA) and kappa(CC)(N), the kappa(HTDMA) / kappa(CC)(N )ratio increased with the SOA mass fraction and this was observed in all investigated single and mixed VOC systems, independent of initial VOC concentrations and sources. For all VOC systems, the mean kappa(HTDMA) of aerosol particles was similar to 25 % lower than the icccN at the beginning of the experiments with inorganic seeds. With the increase of condensed SOA on inorganic seed particles throughout the experiments, the discrepancy of kappa(HTDMA )and kappa(CC)(N )became weaker (down to similar to 0 %) and finally the mean kappa(HTDMA )was similar to 60 % higher than icccN on average when the SOA mass fraction approached similar to 0.8. As indicated by AIOMFAC model simulations, non-ideality alone cannot fully explain the kappa discrepancy at high SOA mass fraction (0.8). A good agreement in icccN between model and observation was achieved by doubling the molecular weight of the model compounds or by reducing the dry particle size in the (CCN) counter. This indicates that the evaporation of semi-volatile organics in the CCN counter together with non-ideality could have led to the observed kappa discrepancy. As a result, the predicted CCN number concentrations from the kappa(HTDMA)and particle number size distribution were similar to 10 % lower than CCN counter measurement on average at the beginning, and further even turned to an overestimation of similar to 20 % on average when the SOA mass fraction was similar to 0.8. This chemical composition-dependent performances of the kappa-Kohler approach on CCN prediction can introduce a variable uncertainty in predicting cloud droplet numbers from the sub-saturated water uptake, the influence of which on models still needs to be investigated.
学科领域	Environmental Sciences; Meteorology & Atmospheric Sciences
语种	英语
WOS研究方向	Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences
WOS记录号	WOS:000776147400001
来源期刊	ATMOSPHERIC CHEMISTRY AND PHYSICS
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/273788
作者单位	University of Manchester; University of Exeter; Swiss Federal Institutes of Technology Domain; ETH Zurich; UK Research & Innovation (UKRI); Natural Environment Research Council (NERC); NERC National Centre for Atmospheric Science; University of Manchester; Qatar Foundation (QF); Hamad Bin Khalifa University-Qatar; Qatar Environment & Energy Research Institute; Swiss Federal Institutes of Technology Domain; Paul Scherrer Institute
推荐引用方式 GB/T 7714	Wang, Yu,Voliotis, Aristeidis,Hu, Dawei,et al. On the evolution of sub- and super-saturated water uptake of secondary oraanic aerosol in chamber experiments from mixed precursors[J],2022,22(6):18.
APA	Wang, Yu.,Voliotis, Aristeidis.,Hu, Dawei.,Shao, Yunqi.,Du, Mao.,...&McFiggans, Gordon.(2022).On the evolution of sub- and super-saturated water uptake of secondary oraanic aerosol in chamber experiments from mixed precursors.ATMOSPHERIC CHEMISTRY AND PHYSICS,22(6),18.
MLA	Wang, Yu,et al."On the evolution of sub- and super-saturated water uptake of secondary oraanic aerosol in chamber experiments from mixed precursors".ATMOSPHERIC CHEMISTRY AND PHYSICS 22.6(2022):18.