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.

<p><strong>Abstract.</strong> 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.</p> <p> 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 (<i>D</i><sub>half</sub><sup>cloud</sup>), 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 (SS<sub>peak</sub>) of a cloud was derived from <i>D</i><sub>half</sub><sup>cloud</sup> 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 SS<sub>peak</sub> 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 SS<sub>peak</sub> ≈ 0.21 %, increasing up to ~ 80 % activated fraction at SS<sub>peak</sub> ≈ 0.5 %. On a single particle basis, BC activation at a certain SS<sub>peak</sub> 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 SS<sub>peak</sub> and, second, variations in BC core size distribution and mean coating thickness are limited in the lower free troposphere in summer.</p>

A new measurement method has been developed that enables an acoustic detection of individual coarse mode particles (aerodynamic particle diameter > 1 µm) by impaction on a piezo transducer. The aerosol is accelerated and each momentum transfer by a particle is measured as a characteristic pulse in the transducer signal whose amplitude is directly proportional to the particle mass. The current single particle mass detection limit is approximately 50 picograms, which corresponds to an aerodynamic particle diameter of ∼5 µm. The measurement technique allows a direct in-situ mass measurement of single coarse mode particles that is unique because it is based on first principles, is relatively simple and less prone to measurement artefacts compared to other methods. This particle mass measurement is independent of assumptions on particle properties like shape, density or refractive index. This technology is of interest for scientific, industrial and health-related monitoring applications as different sources of atmospheric aerosols can be identified via size-resolved mass measurements. Challenges to be overcome include a further lowering of the detection limit, eliminating systematic errors from bouncing phenomena, optimizing the correct mass assignment as well as improving the robustness against sensor vibrations and acoustic noise. In addition, the complete sensor should be portable and affordable. With the future goal to detect submicron particles, coincidence and a reduction of the impactor's cutoff diameter additionally become important issues.

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