Direct quantification of droplet activation of ambient black carbon under water supersaturation

Abstract. 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 single-particle 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 (Dhalfcloud), 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 Dhalfcloud 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 single-particle 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 size-integrated 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 BC-containing particle size and mixing state.

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Droplet activation behaviour of atmospheric black carbon particles in fog as a function of their size and mixing state

Atmospheric Chemistry and Physics ◽

10.5194/acp-19-2183-2019 ◽

2019 ◽

Vol 19 (4) ◽

pp. 2183-2207 ◽

Cited By ~ 9

Author(s):

Ghislain Motos ◽

Julia Schmale ◽

Joel C. Corbin ◽

Marco Zanatta ◽

Urs Baltensperger ◽

...

Keyword(s):

Black Carbon ◽

Single Particle ◽

Radiative Forcing ◽

Mixing State ◽

Scanning Mobility Particle Sizer ◽

Carbon Particles ◽

Kohler Theory ◽

Droplet Activation ◽

Aerosol Cloud Interactions ◽

A Minor

Abstract. Among the variety of particle types present in the atmosphere, black carbon (BC), emitted by combustion processes, is uniquely associated with harmful effects to the human body and substantial radiative forcing of the Earth. Pure BC is known to be non-hygroscopic, but its ability to acquire a coating of hygroscopic organic and inorganic material leads to increased diameter and hygroscopicity, facilitating droplet activation. This affects BC radiative forcing through aerosol–cloud interactions (ACIs) and BC life cycle. To gain insights into these processes, we performed a field campaign in winter 2015–2016 in a residential area of Zurich which aimed at establishing relations between the size and mixing state of BC particles and their activation to form droplets in fog. This was achieved by operating a CCN counter (CCNC), a scanning mobility particle sizer (SMPS), a single-particle soot photometer (SP2) and an aerosol chemical speciation monitor (ACSM) behind a combination of a total- and an interstitial-aerosol inlet. Our results indicate that in the morning hours of weekdays, the enhanced traffic emissions caused peaks in the number fraction of externally mixed BC particles, which do not act as CCN within the CCNC. The very low effective peak supersaturations (SSpeak) occurring in fog (between approximately 0.03 % and 0.06 % during this campaign) restrict droplet activation to a minor fraction of the aerosol burden (around 0.5 % to 1 % of total particle number concentration between 20 and 593 nm) leading to very selective criteria on diameter and chemical composition. We show that bare BC cores are unable to activate to fog droplets at such low SSpeak, while BC particles surrounded by thick coating have very similar activation behaviour to BC-free particles. Using simplified κ-Köhler theory combined with the ZSR mixing rule assuming spherical core–shell particle geometry constrained with single-particle measurements of respective volumes, we found good agreement between the predicted and the directly observed size- and mixing-state-resolved droplet activation behaviour of BC-containing particles in fog. This successful closure demonstrates the predictability of their droplet activation in fog with a simplified theoretical model only requiring size and mixing state information, which can also be applied in a consistent manner in model simulations.

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Droplet activation behaviour of atmospheric black carbon particles in fog as a function of their size and mixing state

10.5194/acp-2018-811 ◽

2018 ◽

Author(s):

Ghislain Motos ◽

Julia Schmale ◽

Joel Christopher Corbin ◽

Marco Zanatta ◽

Urs Baltensperger ◽

...

Keyword(s):

Black Carbon ◽

Single Particle ◽

Radiative Forcing ◽

Cloud Condensation Nuclei ◽

Mixing State ◽

Scanning Mobility Particle Sizer ◽

Carbon Particles ◽

Hygroscopic Properties ◽

Droplet Activation ◽

Aerosol Cloud Interactions

Abstract. Among the variety of particle types present in the atmosphere, black carbon (BC), emitted by combustion processes, is uniquely associated with harmful effects to the human body and substantial radiative forcing of the Earth. Pure BC is known to be non-hygroscopic, but its ability to acquire a coating of hygroscopic organic and inorganic material leads to increased hygroscopicity as well as diameter, facilitating droplet activation. This affects BC radiative forcing through aerosol-cloud interactions (aci) and BC life cycle. To gain insights into these processes, we performed a field campaign in winter 2015/16 in a residential area of Zurich which aimed at distinguishing different particle mixing states regarding hygroscopic properties in the cloud condensation nuclei (CCN)-activated fraction spectrum of urban aerosol and establishing relations between the mixing state of BC and its activation to form droplets in fog. This was achieved by operating a CCN counter (CCNC), a scanning mobility particle sizer (SMPS), a single particle soot photometer (SP2) and an aerosol chemical speciation monitor (ACSM) behind a combination of a total- and an interstitial-aerosol inlet. Our results indicate that, depending on the time of the day, we sampled both heavily aged internally mixed BC from background air advected to the site and freshly emitted externally mixed BC from local or regional traffic sources. During rush hours in the morning of weekdays, we found clear evidence that the enhanced traffic emissions caused peaks in the number fraction of externally mixed BC particles which do not act as CCN within the CCNC. The mixing state of BC particles was also found to play a key role in their ability to form fog droplets. The very low effective peak supersaturations (SSpeak) occurring in fog (between approximately 0.03 and 0.06 % during this campaign) restrict droplet activation to a minor fraction of the aerosol burden (around 0.5 to 1 % of total particle number concentration between 20 and 593 nm) leading to very selective criteria on diameter and chemical composition. We show that bare BC cores are unable to activate to fog droplets at such low SSpeak, while BC particles surrounded by thick coating have a very similar activation behavior as BC-free particles. The threshold coating thickness required for activation was shown to decrease with increasing BC core size. Using simplified κ-Köhler theory combined with the ZSR mixing rule assuming spherical core-shell particle geometry constrained with single particle measurements of respective volumes, we found good agreement between the predicted and the directly observed size and mixing state resolved droplet activation behaviour of BC-containing particles in fog. This successful closure demonstrates the predictability of their droplet activation in fog with a simplified theoretical model only requiring size and mixing state information, which can also be applied in a consistent manner in model simulations.

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Supplementary material to "Cloud droplet activation properties and scavenged fraction of black carbon in liquid-phase clouds at the high-alpine research station Jungfraujoch (3580 m a.s.l.)"

10.5194/acp-2018-1054-supplement ◽

2018 ◽

Author(s):

Ghislain Motos ◽

Julia Schmale ◽

Joel C. Corbin ◽

Robin Modini ◽

Nadine Karlen ◽

...

Keyword(s):

Liquid Phase ◽

Black Carbon ◽

Cloud Droplet ◽

Research Station ◽

Supplementary Material ◽

Droplet Activation ◽

Alpine Research

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Cloud droplet activation properties and scavenged fraction of black carbon in liquid-phase clouds at the high-alpine research station Jungfraujoch (3580 m a.s.l.)

10.5194/acp-2018-1054 ◽

2018 ◽

Cited By ~ 1

Author(s):

Ghislain Motos ◽

Julia Schmale ◽

Joel C. Corbin ◽

Robin Modini ◽

Nadine Karlen ◽

...

Keyword(s):

Black Carbon ◽

Single Particle ◽

Aerosol Particles ◽

Cloud Droplet ◽

Water Soluble ◽

High Mountain ◽

Research Station ◽

Core Size ◽

Cloud Droplets ◽

Droplet Activation

Abstract. Liquid clouds form by condensation of water vapour on aerosol particles in the atmosphere. Even black carbon (BC) particles, which are known to be little 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 mountain 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 single particle 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 (Dhalfcloud), 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 Dhalfcloud 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. Fifty percent of the BC-containing particles with a BC mass equivalent core diameter of 90 nm were activated in clouds with SSpeak ≈ 0.21 %, increasing up to ~ 80 % activated fraction at SSpeak ≈ 0.5 %. On a single particle 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 size integrated 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.

Download Full-text