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On time scales that are long compared to the phase relaxation time, a quasi-steady supersaturation sqs is expected to exist in clouds. On shorter time scales, however, turbulent fluctuations of temperature and water vapor concentration should generate fluctuations in supersaturation. The variability of temperature, water vapor, and supersaturation has been measured in situ with submeter resolution in warm, continental, shallow cumulus clouds. Several cumuli with horizontal extents of order 100 m were sampled during their first appearance and development to depths of ~100 m in a growing boundary layer. Fluctuations of the saturation ratio are observed to be approximately normally distributed with standard deviations on the order of 1%. This variability is almost one order of magnitude larger than sqs calculated using simultaneous measurements of the vertical velocity component and the droplet size distribution. It is argued that, depending on the ratio of the phase relaxation and the turbulent mixing time, substantial fluctuations in the supersaturation field can exist on small spatial scales, centered on sqs for the mean state. The observations also suggest that, on larger scales, fluctuations of the supersaturation field are damped by cloud droplet growth. Droplets with diameters of up to 20 μm were observed in the shallow cumulus clouds, whereas the adiabatic diameter was less than 10 μm. Such large droplets may be explained by a few droplets experiencing the highest observed supersaturations for a certain time. Consequences for aerosol activation and droplet size dispersion in a highly fluctuating supersaturation field are briefly discussed.

The influence of aerosol concentration on the cloud-droplet size distribution is investigated in a laboratory chamber that enables turbulent cloud formation through moist convection. The experiments allow steady-state microphysics to be achieved, with aerosol input balanced by cloud-droplet growth and fallout. As aerosol concentration is increased, the cloud-droplet mean diameter decreases, as expected, but the width of the size distribution also decreases sharply. The aerosol input allows for cloud generation in the limiting regimes of fast microphysics (τc < τt ) for high aerosol concentration, and slow microphysics (τc > τt ) for low aerosol concentration; here, τc is the phase-relaxation time and τt is the turbulence-correlation time. The increase in the width of the droplet size distribution for the low aerosol limit is consistent with larger variability of supersaturation due to the slow microphysical response. A stochastic differential equation for supersaturation predicts that the standard deviation of the squared droplet radius should increase linearly with a system time scale defined as τ s − 1 = τ c − 1 + τ t − 1 , and the measurements are in excellent agreement with this finding. The result underscores the importance of droplet size dispersion for aerosol indirect effects: increasing aerosol concentration changes the albedo and suppresses precipitation formation not only through reduction of the mean droplet diameter but also by narrowing of the droplet size distribution due to reduced supersaturation fluctuations. Supersaturation fluctuations in the low aerosol/slow microphysics limit are likely of leading importance for precipitation formation.

Optical properties and precipitation efficiency of atmospheric clouds are largely determined by turbulent mixing with their environment. When cloud liquid water is reduced upon mixing, droplets may evaporate uniformly across the population or, in the other extreme, a subset of droplets may evaporate completely, leaving the remaining drops unaffected. Here, we use airborne holographic imaging to visualize the spatial structure and droplet size distribution at the smallest turbulent scales, thereby observing their response to entrainment and mixing with clear air. The measurements reveal that turbulent clouds are inhomogeneous, with sharp transitions between cloud and clear air properties persisting to dissipative scales (<1 centimeter). The local droplet size distribution fluctuates strongly in number density but with a nearly unchanging mean droplet diameter.

The entrainment of clear air and its subsequent mixing with a filament of cloudy air, as occurs at the edge of a cloud, is studied in three-dimensional direct numerical simulations that combine the Eulerian description of the turbulent velocity, temperature, and vapor fields with a Lagrangian cloud droplet ensemble. Forced and decaying turbulence is considered, such as when the dynamics around the filament is driven by larger-scale eddies or during the final period of the life cycle of a cloud. The microphysical response depicted in nd − 〈r3〉 space (where nd and r are droplet number density and radius, respectively) shows characteristics of both homogeneous and inhomogeneous mixing, depending on the Damköhler number. The transition from inhomogeneous to homogeneous mixing leads to an offset of the homogeneous mixing curve to larger dilution fractions. The response of the system is governed by the smaller of the single droplet evaporation time scale and the bulk phase relaxation time scale. Variability within the nd − 〈r3〉 space increases with decreasing sample volume, especially during the mixing transients. All of these factors have implications for the interpretation of measurements in clouds. The qualitative mixing behavior changes for forced versus decaying turbulence, with the latter yielding remnant patches of unmixed cloud and stronger fluctuations. Buoyancy due to droplet evaporation is observed to play a minor role in the mixing for the present configuration. Finally, the mixing process leads to the transient formation of a pronounced nearly exponential tail of the probability density function of the Lagrangian supersaturation, and a similar tail emerges in the droplet size distribution under inhomogeneous conditions.

Turbulence is ubiquitous in atmospheric clouds, which have enormous turbulence Reynolds numbers owing to the large range of spatial scales present. Indeed, the ratio of energy-containing and dissipative length scales is on the order of 10 5 for a typical convective cloud, with a corresponding large-eddy Reynolds number on the order of 10 6 to 10 7 . A characteristic trait of high-Reynolds-number turbulence is strong intermittency in energy dissipation, Lagrangian acceleration, and scalar gradients at small scales. Microscale properties of clouds are determined to a great extent by thermodynamic and fluid-mechanical interactions between droplets and the surrounding air, all of which take place at small spatial scales. Furthermore, these microscale properties of clouds affect the efficiency with which clouds produce rain as well as the nature of their interaction with atmospheric radiation and chemical species. It is expected, therefore, that fine-scale turbulence is of direct importance to the evolution of, for example, the droplet size distribution in a cloud. In general, there are two levels of interaction that are considered in this review: ( a ) the growth of cloud droplets by condensation and ( b ) the growth of large drops through the collision and coalescence of cloud droplets. Recent research suggests that the influence of fine-scale turbulence on the condensation process may be limited, although several possible mechanisms have not been studied in detail in the laboratory or the field. There is a growing consensus, however, that the collision rate and collision efficiency of cloud droplets can be increased by turbulence-particle interactions. Adding strength to this notion is the growing experimental evidence for droplet clustering at centimeter scales and below, most likely due to strong fluid accelerations in turbulent clouds. Both types of interaction, condensation and collision-coalescence, remain open areas of research with many possible implications for the physics of atmospheric clouds.

Cloud droplet size distributions (CDSDs), which are related to cloud albedo and rain formation, are usually broader in warm clouds than predicted from adiabatic parcel calculations. We investigate a mechanism for the CDSD broadening using a moving-size-grid cloud parcel model that considers the condensational growth of cloud droplets formed on polydisperse, submicrometer aerosols in an adiabatic cloud parcel that undergoes vertical oscillations, such as those due to cloud circulations or turbulence. Results show that the CDSD can be broadened during condensational growth as a result of Ostwald ripening amplified by droplet deactivation and reactivation, which is consistent with early work. The relative roles of the solute effect, curvature effect, deactivation and reactivation on CDSD broadening are investigated. Deactivation of smaller cloud droplets, which is due to the combination of curvature and solute effects in the downdraft region, enhances the growth of larger cloud droplets and thus contributes particles to the larger size end of the CDSD. Droplet reactivation, which occurs in the updraft region, contributes particles to the smaller size end of the CDSD. In addition, we find that growth of the largest cloud droplets strongly depends on the residence time of cloud droplet in the cloud rather than the magnitude of local variability in the supersaturation fluctuation. This is because the environmental saturation ratio is strongly buffered by numerous smaller cloud droplets. Two necessary conditions for this CDSD broadening, which generally occur in the atmosphere, are as follows: (1) droplets form on aerosols of different sizes, and (2) the cloud parcel experiences upwards and downwards motions. Therefore we expect that this mechanism for CDSD broadening is possible in real clouds. Our results also suggest it is important to consider both curvature and solute effects before and after cloud droplet activation in a cloud model. The importance of this mechanism compared with other mechanisms on cloud properties should be investigated through in situ measurements and 3-D dynamic models.

The helicopter-borne instrument payload known as the Airborne Cloud Turbulence Observation System (ACTOS) was used to study the entrainment and mixing processes in shallow warm cumulus clouds. The characteristics of the mixing process are determined by the Damköhler number, defined as the ratio of the mixing and a thermodynamic reaction time scale. The definition of the reaction time scale is refined by investigating the relationship between the droplet evaporation time and the phase relaxation time. Following arguments of classical turbulence theory, it is concluded that the description of the mixing process through a single Damköhler number is not sufficient and instead the concept of a transition length scale is introduced. The transition length scale separates the inertial subrange into a range of length scales for which mixing between ambient dry and cloudy air is inhomogeneous, and a range for which the mixing is homogeneous. The new concept is tested on the ACTOS dataset. The effect of entrained subsaturated air on the droplet number size distribution is analyzed using mixing diagrams correlating droplet number concentration and droplet size. The data suggest that homogeneous mixing is more likely to occur in the vicinity of the cloud core, whereas inhomogeneous mixing dominates in more diluted cloud regions. Paluch diagrams are used to support this hypothesis. The observations suggest that homogeneous mixing is favored when the transition length scale exceeds approximately 10 cm. Evidence was found that suggests that under certain conditions mixing can lead to enhanced droplet growth such that the largest droplets are found in the most diluted cloud regions.

Collisional growth of cloud droplets is an essential yet uncertain process for drizzle and precipitation formation. To improve the quantitative understanding of this key component of cloud‐aerosol‐turbulence interactions, observational studies of collision‐coalescence in a controlled laboratory environment are needed. In an existing convection‐cloud chamber (the Pi Chamber), collisional growth is limited by low liquid water content and short droplet residence times. In this work, we use numerical simulations to explore various configurations of a convection‐cloud chamber that may intensify collision‐coalescence. We employ a large‐eddy simulation (LES) model with a size‐resolved (bin) cloud microphysics scheme to explore how cloud properties and the intensity of collision‐coalescence are affected by the chamber size and aspect ratio, surface roughness, side‐wall wetness, side‐wall temperature arrangement, and aerosol injection rate. Simulations without condensation and evaporation within the domain are first performed to explore the turbulence dynamics and wall fluxes. The LES wall fluxes are used to modify the Scalar Flux‐budget Model, which is then applied to demonstrate the need for non‐uniform side‐wall temperature (two side walls as warm as the bottom and the two others as cold as the top) to maintain high supersaturation in a tall chamber. The results of LES with full cloud microphysics reveal that collision‐coalescence is greatly enhanced by employing a taller chamber with saturated side walls, non‐uniform side‐wall temperature, and rough surfaces. For the conditions explored, although lowering the aerosol injection rate broadens the droplet size distribution, favoring collision‐coalescence, the reduced droplet number concentration decreases the frequency of collisions. Plain Language Summary A convection‐cloud chamber is useful in understanding how turbulence affects the interaction between aerosols and cloud droplets. The current convection‐cloud chamber (the Pi Chamber) is likely too small to explore how turbulence affects the collision‐coalescence among cloud droplets. To see whether collisional growth may be observable in a larger cloud chamber, we use numerical simulations to model the cloud droplet size distributions under several different configurations of the cloud chamber. The results suggest that the likelihood of detectable collisional growth increases significantly in a tall chamber with two warm and two cold saturated side walls and rough wall surfaces. Key Points Collision‐coalescence effects on a steady‐state droplet size distribution are stronger in a taller chamber Wet side walls are essential for maintaining cloud liquid water in a chamber with a low width‐to‐height aspect ratio Rougher surfaces increase surface heat and moisture fluxes, leading to larger liquid water content that promotes collision‐coalescence

Experiments in the Pi Convection‐Cloud Chamber conducted by systematically changing the diameter of injected dry aerosol particles while holding the temperature difference constant demonstrate that dry diameter strongly influences the onset of haze‐dominated conditions. Two factors contribute: the system becomes water‐limited, resulting in reduction of supersaturation by growing aerosol particles to the activation diameter; and the activation process becomes kinetically limited. Dry aerosol diameter exerts a strong influence on activation time, with a power‐law exponent of 9/2 $9/2$. Kinetically limited activation occurs when the ratio of the activation and droplet residence times is greater than unity. The findings demonstrate that a haze‐dominated state, where cloud formation is suppressed, can be achieved not only with weak supersaturation forcing and high aerosol concentration but also with large, hygroscopic aerosol particles. These results have implications for cloud formation in polluted environments, fog development near the ocean, and hygroscopic cloud seeding.

The effect of aerosols on the properties of clouds is a large source of uncertainty in predictions of weather and climate. These aerosol‐cloud interactions depend critically on the ability of aerosol particles to form cloud droplets. A challenge in modeling aerosol‐cloud interactions is the representation of interactions between turbulence and cloud microphysics. Turbulent mixing leads to small‐scale fluctuations in water vapor and temperature that are unresolved in large‐scale atmospheric models. To quantify the impact of turbulent fluctuations on cloud condensation nuclei (CCN) activation, we used a high‐resolution Large Eddy Simulation of a convective cloud chamber to drive particle‐based cloud microphysics simulations. We show small‐scale fluctuations strongly impact CCN activity. Once activated, the relatively long timescales of evaporation compared to fluctuations causes droplets to persist in subsaturated regions, which further increases droplet concentrations. Plain Language Summary Increases in cloud droplet number concentrations from human emissions of aerosol particles modify cloud properties, which strongly impacts Earth's energy balance. Large Eddy Simulations and Earth System Models are used to quantify these aerosol‐cloud interactions, but the spatial and temporal resolution of these models is too coarse to represent the impact of turbulence at the smallest scales. In this study, we show that small‐scale turbulent fluctuations lead to cloud droplet formation even when air is, on average, subsaturated, which would be impossible in conventional models of cloud microphysics. Our findings suggest that models that neglect turbulent fluctuations in supersaturation will underestimate cloud condensation nuclei activity under specific supersaturation regimes, which will may lead to error in modeled cloud properties. Key Points Small‐scale turbulence leads to variability in the supersaturation experienced by aerosol particles and cloud droplets within clouds Turbulent fluctuations increase cloud droplet formation at low supersaturation levels in comparison with uniform environmental conditions Atmospheric models that neglect supersaturation variability due to turbulence may underestimate the number concentration of cloud droplets