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DOI10.5194/acp-19-3833-2019
Cloud droplet activation properties and scavenged fraction of black carbon in liquid-phase clouds at the high-alpine research station Jungfraujoch (3580ma.s.l.)
Motos G.; Schmale J.; Corbin J.C.; Modini R.L.; Karlen N.; Bertò M.; Baltensperger U.; Gysel-Beer M.
发表日期2019
ISSN16807316
起始页码3833
结束页码3855
卷号19期号:6
英文摘要Liquid clouds form by condensation of water vapour on aerosol particles in the atmosphere. Even black carbon (BC) particles, which are known to be slightly hygroscopic, have been shown to readily form cloud droplets once they have acquired water-soluble coatings by atmospheric aging processes. Accurately simulating the life cycle of BC in the atmosphere, which strongly depends on the wet removal following droplet activation, has recently been identified as a key element for accurate prediction of the climate forcing of BC. Here, to assess BC activation in detail, we performed in situ measurements during cloud events at the Jungfraujoch high-altitude station in Switzerland in summer 2010 and 2016. Cloud droplet residual and interstitial (unactivated) particles as well as the total aerosol were selectively sampled using different inlets, followed by their physical characterization using scanning mobility particle sizers (SMPSs), multi-angle absorption photometers (MAAPs) and a singleparticle soot photometer (SP2). By calculating cloud droplet activated fractions with these measurements, we determined the roles of various parameters on the droplet activation of BC. The half-rise threshold diameter for droplet activation (Dhalf cloud), i.e. the size above which aerosol particles formed cloud droplets, was inferred from the aerosol size distributions measured behind the different inlets. The effective peak supersaturation (SSpeak) of a cloud was derived from Dhalf cloud by comparing it to the supersaturation dependence of the threshold diameter for cloud condensation nuclei (CCN) activation measured by a CCN counter (CCNC). In this way, we showed that the mass-based scavenged fraction of BC strongly correlates with that of the entire aerosol population because SSpeak modulates the critical size for activation of either particle type. A total of 50 % of the BC-containing particles with a BC mass equivalent core diameter of 90 nm was activated in clouds with SSpeak ≈0:21 %, increasing up to ∼ 80 % activated fraction at SSpeak ≈0:50 %. On a singleparticle basis, BC activation at a certain SSpeak is controlled by the BC core size and internally mixed coating, which increases overall particle size and hygroscopicity. However, the resulting effect on the population averaged and on the sizeintegrated BC scavenged fraction by mass is small for two reasons: first, acquisition of coatings only matters for small cores in clouds with low SSpeak; and, second, variations in BC core size distribution and mean coating thickness are limited in the lower free troposphere in summer. Finally, we tested the ability of a simplified theoretical model, which combines the κ-Köhler theory with the Zdanovskii-Stokes-Robinson (ZSR) mixing rule under the assumptions of spherical core-shell particle geometry and surface tension of pure water, to predict the droplet activation behaviour of BC-containing particles in real clouds. Predictions of BC activation constrained with SSpeak and measured BC-containing particle size and mixing state were compared with direct cloud observations. These predictions achieved closure with the measurements for the particle size ranges accessible to our instrumentation, that is, BC core diameters and total particle diameters of approximately 50 and 180 nm, respectively. This clearly indicates that such simplified theoretical models provide a sufficient description of BC activation in clouds, as previously shown for activation occurring in fog at lower supersaturation and also shown in laboratory experiments under controlled conditions. This further justifies application of such simplified theoretical approaches in regional and global simulations of BC activation in clouds, which include aerosol modules that explicitly simulate BCcontaining particle size and mixing state. © 2019 Author(s).
语种英语
scopus关键词aerosol; alpine environment; black carbon; cloud droplet; in situ measurement; particle size; scavenging (chemistry); Switzerland
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/144547
作者单位Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, 5232, Switzerland; Metrology Research Centre, National Research Council Canada, 1200 Montreal Road, Ottawa, ON K1A 0R6, Canada; Institute for Sensors and Electronics, University of Applied Sciences (FHNW), Windisch, Switzerland
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Motos G.,Schmale J.,Corbin J.C.,et al. Cloud droplet activation properties and scavenged fraction of black carbon in liquid-phase clouds at the high-alpine research station Jungfraujoch (3580ma.s.l.)[J],2019,19(6).
APA Motos G..,Schmale J..,Corbin J.C..,Modini R.L..,Karlen N..,...&Gysel-Beer M..(2019).Cloud droplet activation properties and scavenged fraction of black carbon in liquid-phase clouds at the high-alpine research station Jungfraujoch (3580ma.s.l.).Atmospheric Chemistry and Physics,19(6).
MLA Motos G.,et al."Cloud droplet activation properties and scavenged fraction of black carbon in liquid-phase clouds at the high-alpine research station Jungfraujoch (3580ma.s.l.)".Atmospheric Chemistry and Physics 19.6(2019).
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