Prior observations have documented the process of cloud cleansing, through which cloudy, polluted air from a continent is slowly transformed into cloudy, clean air typical of a maritime environment. During that process, cloud albedo changes gradually, followed by a sudden reduction in cloud fraction and albedo as drizzle forms and convection changes from closed to open cellular. Experiments in a cloud chamber that generates a turbulent environment show a similar cloud cleansing process followed by rapid cloud collapse. Observations of (1) cloud droplet size distribution, (2) interstitial aerosol size distribution, (3) cloud droplet residual size distribution, and (4) water vapor supersaturation are all consistent with the hypothesis that turbulent fluctuations of supersaturation accelerate the cloud cleansing process and eventual cloud collapse. Decay of the interstitial aerosol concentration occurs slowly at first then more rapidly. The accelerated cleansing occurs when the cloud phase relaxation time exceeds the turbulence correlation time.

Aerosol indirect effects are one of the leading contributors to cloud radiative properties relevant to climate. Aerosol particles become cloud droplets when the ambient relative humidity (saturation ratio) exceeds a critical value, which depends on the particle size and chemical composition. In the traditional formulation of this problem, only average, uniform saturation ratios are considered. Using experiments and theory, we examine the effects of fluctuations, produced by turbulence. Our measurements, from a multiphase, turbulent cloud chamber, show a clear transition from a regime in which the mean saturation ratio dominates to one in which the fluctuations determine cloud properties. The laboratory measurements demonstrate cloud formation in mean-subsaturated conditions (i.e., relative humidity <100%) in the fluctuation-dominant activation regime. The theoretical framework developed to interpret these measurements predicts a transition from a mean- to a fluctuation-dominated regime, based on the relative values of the mean and standard deviation of the environmental saturation ratio and the critical saturation ratio at which aerosol particles activate or become droplets. The theory is similar to the concept of stochastic condensation and can be used in the context of the atmosphere to explore the conditions under which droplet activation is driven by fluctuations as opposed to mean supersaturation. It provides a basis for future development of cloud droplet activation parameterizations that go beyond the internally homogeneous parcel calculations that have been used in the past.

Soot particles form during combustion of carbonaceous materials and impact climate and air quality. When freshly emitted, they are typically fractal-like aggregates. After atmospheric aging, they can act as cloud condensation nuclei, and water condensation or evaporation restructure them to more compact aggregates, affecting their optical, aerodynamic, and surface properties. Here we survey the morphology of ambient soot particles from various locations and different environmental and aging conditions. We used electron microscopy and show extensive soot compaction after cloud processing. We further performed laboratory experiments to simulate atmospheric cloud processing under controlled conditions. We find that soot particles sampled after evaporating the cloud droplets, are significantly more compact than freshly emitted and interstitial soot, confirming that cloud processing, not just exposure to high humidity, compacts soot. Our findings have implications for how the radiative, surface, and aerodynamic properties, and the fate of soot particles are represented in numerical models.

What concentration of ice‐nucleating particles is required to completely glaciate a typical atmospheric supercooled liquid cloud? This seemingly esoteric question has far reaching implications, as the ratio of liquid to ice in these clouds governs, for example, their influence on Earth's radiation budget and their precipitation efficiency. Microphysical properties of steady‐state mixed‐phase clouds formed in a laboratory convection chamber are observed using digital holography. It is observed that the ratio of ice to total water content of steady‐state mixed‐phase clouds is determined by the concentration of ice‐nucleating aerosol particles. Existing theory is adapted to show such clouds result from a balance between the thermodynamic forcing (i.e., the source of excess water vapor that is condensing to liquid and ice) and the number and size of particles that become ice (i.e., the ice integral radius). The measurements quantitatively support the Korolev‐Mazin conditions for existence of mixed‐phase clouds.

Aerosol particles, cloud droplets, and ice crystals, coupled through the supersaturation field, play an important role in the buoyancy and life cycle of convective clouds. This letter reports laboratory observations of copious cloud droplets and ice crystals formed in the wake of a warm, falling water drop, which is a laboratory surrogate for a relatively warm hydrometeor in atmospheric clouds, such as a graupel particle in the wet growth regime. Aerosols were activated in the regions of very high supersaturation due to mixing in the wake. A mechanism is explored for attaining very high supersaturations capable of activating significant fractions of the interstitial aerosols within the lifetime of a convective cloud. The latent heat released from the activation of interstitial aerosols and subsequent growth may provide an additional source of buoyancy for cloud invigoration and may lead to larger concentrations of ice crystals. Plain Language SummaryHail or other large icy hydrometeors like graupel fall through clouds, leaving regions of disturbed turbulent air in their wake. Because graupel particles are very likely to be warm or cold, relative to their surroundings, numerous new cloud droplets and even ice crystals can form in the disturbed air. The heat associated with the condensation of water vapor onto these newly formed droplets or crystals could provide a significant boost to the cloud's buoyancy. Calculations suggest that this mechanism could expose regions of convective clouds to high supersaturations in tens of minutes, providing a source of invigoration and higher concentrations of ice crystals.