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Abstract. This study delves into the small-scale temperature structure inside the turbulent convection Π Chamber under three temperature differences (10, 15, and 20 K) at Rayleigh number Ra∼109 and Prandtl number Pr≈0.7. We performed high-frequency measurements (2 kHz) with the UltraFast Thermometer (UFT) at selected points along the vertical axis. The miniaturized design of the sensor with a resistive platinum-coated tungsten wire, 2.5 µm thick and 3 mm long, mounted on a miniature wire probe, allowed for vertically undisturbed temperature profiling through the chamber's depth spanning from 8 cm above the bottom to 5 cm below the top. The collected data, consisting of 19 and 3 min time series, were used to investigate the variability of the temperature field within the chamber, aiming to better address scientific questions related to its primary objective: understanding small-scale aerosol–cloud interactions. The analyses reveal substantial variability in both variance and skewness of temperature distributions near the top and bottom plates and in the bulk (central) region, which were linked to local thermal plume dynamics. We also identified three spectral regimes termed “inertial range” (slopes of ∼-7/5), “transition range” (slopes of ∼-3), and “dissipative range”, characterized by slopes of ∼-7. Furthermore, the analysis showed a power law relationship between the periodicity of large-scale circulation (LSC) and the temperature difference. Notably, the experimental results are in good agreement with direct numerical simulation (DNS) conducted under similar thermodynamic conditions, illustrating a comparative analysis of this nature. 

Impacts of aerosol particles on clouds, precipitation, and climate remain one of the significant uncertainties in climate change. Aerosol particles entrained at cloud top and edge can affect cloud microphysical and macrophysical properties, but the process is still poorly understood. Here we investigate the cloud microphysical responses to the entrainment of aerosol-laden air in the Pi convection-cloud chamber. Results show that cloud droplet number concentration increases and mean radius of droplets decreases, which leads to narrower droplet size distribution and smaller relative dispersion. These behaviors are generally consistent with the scenario expected from the first aerosol-cloud indirect effect for a constant liquid water content (L). However, L increases significantly in these experiments. Such enhancement of L can be understood as suppression of droplet sedimentation removal due to small droplets. Further, an increase in aerosol concentration from entrainment reduces the effective radius and ultimately increases cloud optical thickness and cloud albedo, making the clouds brighter. These findings are of relevance to the entrainment interface at stratocumulus cloud top, where modeling studies have suggested sedimentation plays a strong role in regulating L. Therefore, the results provide insights into the impacts of entrainment of aerosol-laden air on cloud, precipitation, and climate. 

Entrainment of subsaturated air into a cloud can influence its optical and microphysical properties in various ways, depending on the droplet evaporation and turbulent mixing time scales. Previous experiments in the Pi convection-cloud chamber have revealed that, given a fixed entrained air property, the mixing of entrained subsaturated air results in complete evaporation of some cloud droplets, with the rest remaining unchanged. This is a signature of inhomogeneous mixing. While comparing the results of entrainment with varying air properties, the mixing signature appears as if the subsaturated air is well mixed with the cloud to evenly reduce the droplets’ size. In other words, taken together, the experiments appear to have the signature of homogeneous mixing. To explore these results in a greater depth, we conduct large-eddy simulations combined with a bin microphysics scheme. Our results reproduce the similar signatures of inhomogeneous and homogeneous mixing, implying that LES can resolve the inhomogeneous mixing when the grid spacing is smaller than the entrained air parcel. Additionally, we observe that increasing the aerosol injection rate enhances the signature of inhomogeneous mixing, while coarser grid spacing diminishes it. Finally, the change in wall fluxes in response to various entrained air properties confirms that the homogeneous signature seen in the analysis of an ensemble of simulations is the result of various equilibrium states. This further strengthens the suggestion that the homogeneous mixing signature found in aircraft observations near the cloud top may result from combining entrainment events of different intensities, possibly caused by various-sized eddies. Significance StatementLarge-eddy simulation and size-resolved microphysics can resolve time scales for turbulent mixing and evaporation and, therefore, are well suited for reproducing, extending, and interpreting the entrainment experiment in the Pi convection-cloud chamber. Our simulation results confirm (i) the inhomogeneous mixing signature for an individual entrainment event and (ii) the appearance of homogeneous mixing in an ensemble of entrainment episodes. Furthermore, we demonstrate that the inhomogeneous mixing signature is more pronounced in a polluted cloud, but coarser grid spacing in simulations may compromise the accuracy of this signature. Last, the homogeneous mixing signature results from various equilibrium states established for different entrainment intensities and adjusted wall fluxes, which are challenging to measure experimentally but can be easily analyzed in the simulations. 

Abstract Cloud formation in the Pi Convection–Cloud Chamber is achieved via ionization in humid conditions, without the injection of aerosol particles to serve as cloud condensation nuclei (CCN). Abundant ions, turbulence, and supersaturated water vapor combine to produce new particles, which grow to become CCN sized and eventually are activated to form clouds. Coupling between the new particle formation and cloud droplets causes predator-prey type oscillations in aerosol and droplet concentrations under turbulent conditions. Leading terms are identified in the budgets for Aitken and accumulation mode aerosols and for cloud droplets. The cloud coupling is proposed to be a result of cloud-induced runaway CCN production through aerosol scavenging. The experiments suggest potential applications to marine cloud brightening, in which ions rather than sea-salt aerosols are generated. 

Abstract. Mixed-phase clouds affect precipitation and radiation forcing differently from liquid and ice clouds, posing greater challenges to their representation in numerical simulations. Recent laboratory experiments using the Pi Cloud Chamber explored cloud glaciation conditions based on increased injection of ice nucleating particles. In this study, we use two approaches to reproduce the results of the laboratory experiments: a bulk scalar mixing model and large-eddy simulation (LES) with bin microphysics. The first approach assumes a well-mixed domain to provide an efficient assessment of the mean cloud properties for a wide range of conditions. The second approach resolves the energy-carrying turbulence, the particle size distribution, and their spatial distribution to provide more details. These modeling approaches enable a separate and detailed examination of liquid and ice properties, which is challenging in the laboratory. Both approaches demonstrate that, with an increased ice number concentration, the flow and microphysical properties exhibit the same changes in trends. Additionally, both approaches show that the ice integral radius reaches the theoretical glaciation threshold when the cloud is subsaturated with respect to liquid water. The main difference between the results of the two approaches is that the bulk model allows for the complete glaciation of the cloud. However, LES reveals that, in a dynamic system, the cloud is not completely glaciated because liquid water droplets are continuously produced near the warm lower boundary and subsequently mixed into the chamber interior. These results highlight the importance of the ice mass fraction in distinguishing the mixed phase and ice clouds. 

Abstract. Mixed-phase clouds affect precipitation and radiation differently from liquid and ice clouds, posing greater challenges to their representation in numerical simulations. Recent laboratory experiments using the Pi Cloud Chamber explored cloud glaciation conditions based on increased injection of ice-nucleating particles. In this study, we use two approaches to reproduce the results of the laboratory experiments: a bulk scalar mixing model and large-eddy simulation (LES) with bin microphysics. The first approach assumes a well-mixed domain to provide an efficient assessment of the mean cloud properties for a wide range of conditions. The second approach resolves the energy-carrying turbulence, the particle size distribution, and their spatial distribution to provide more details. These modeling approaches enable a separate and detailed examination of liquid and ice properties, which is challenging in the laboratory. Both approaches demonstrate that, with an increased ice number concentration, the flow and microphysical properties exhibit the same changes in trends. Additionally, both approaches show that the ice integral radius reaches the theoretical glaciation threshold when the cloud is subsaturated with respect to liquid water. The main difference between the results of the two approaches is that the bulk model allows for the complete glaciation of the cloud. However, LES reveals that, in a dynamic system, the cloud is not completely glaciated as liquid water droplets are continuously produced near the warm lower boundary and subsequently mixed into the chamber interior. These results highlight the importance of the ice mass fraction in distinguishing the mixed-phase clouds and ice clouds. 

Abstract. Heterogeneous ice nucleation is thought to be the primary pathway for the formation of ice in mixed-phase clouds, with the number of active ice-nucleating particles (INPs) increasing rapidly with decreasing temperature. Here, molecular-dynamics simulations of heterogeneous ice nucleation demonstrate that the ice nucleation rate is also sensitive to pressure and that negative pressure within supercooled water shifts freezing temperatures to higher temperatures. Negative pressure, or tension, occurs naturally in water capillary bridges and pores and can also result from water agitation. Capillary bridge simulations presented in this study confirm that negative Laplace pressure within the water increases heterogeneous-freezing temperatures. The increase in freezing temperatures with negative pressure is approximately linear within the atmospherically relevant range of 1 to −1000 atm. An equation describing the slope depends on the latent heat of freezing and the molar volume difference between liquid water and ice. Results indicate that negative pressures of −500 atm, which correspond to nanometer-scale water surface curvatures, lead to a roughly 4 K increase in heterogeneous-freezing temperatures. In mixed-phase clouds, this would result in an increase of approximately 1 order of magnitude in active INP concentrations. The findings presented here indicate that any process leading to negative pressure in supercooled water may play a role in ice formation, consistent with experimental evidence of enhanced ice nucleation due to surface geometry or mechanical agitation of water droplets. This points towards the potential for dynamic processes such as contact nucleation and droplet collision or breakup to increase ice nucleation rates through pressure perturbations. 

A minimalist model of microphysical properties in cloudy Rayleigh-Bénard convection is developed based on mass and number balances for cloud droplets growing by vapor condensation. The model is relevant to a turbulent mixed-layer in which a steady forcing of supersaturation can be defined, e.g., a model of the cloudy boundary layer or a convection-cloud chamber. The model assumes steady injection of aerosol particles that are activated to form cloud droplets, and the removal of cloud droplets through sedimentation. Simplifying assumptions include the consideration of mean properties in steady state, neglect of coalescence growth, and no detailed representation of the droplet size distribution. Closed-form expressions for cloud droplet radius, number concentration, and liquid water content are derived. Limits of fast and slow microphysics, compared to the turbulent mixing time scale, are explored, and resulting expressions for the scaling of microphysical properties in fast and slow regimes are obtained. Scaling of microphysics with layer thickness is also explored, suggesting that liquid water content and cloud droplet number concentration increase, and mean droplet radius decreases with increasing layer thickness. Finally, the analytical model is shown to compare favorably to solutions of the fully-coupled set of governing ordinary differential equations that describe the system, and the predicted power law for liquid water mixing ratio versus droplet activation rate is observed to be consistent with measurements from the Pi convection-cloud chamber. 

Abstract This study presents the first model intercomparison of aerosol‐cloud‐turbulence interactions in a controlled cloudy Rayleigh‐Bénard Convection chamber environment, utilizing the Pi Chamber at Michigan Technological University. We analyzed simulated cloud chamber‐averaged statistics of microphysics and thermodynamics in a warm‐phase, cloudy environment under steady‐state conditions at varying aerosol injection rates. Simulation results from seven distinct models (DNS, LES, and a 1D turbulence model) were compared. Our findings demonstrate that while all models qualitatively capture observed trends in droplet number concentration, mean radius, and droplet size distributions at both high and low aerosol injection rates, significant quantitative differences were observed. Notably, droplet number concentrations varied by over two orders of magnitude between models for the same injection rates, indicating sensitivities to the model treatments in droplet activation and removal and wall fluxes. Furthermore, inconsistencies in vertical relative humidity profiles and in achieving steady‐state liquid water content suggest the need for further investigation into the mechanisms driving these variations. Despite these discrepancies, the models generally reproduced consistent power‐law relationships between the microphysical variables. This model intercomparison underscores the importance of controlled cloud chamber experiments for validating and improving cloud microphysical parameterizations. Recommendations for future modeling studies are also highlighted, including constraining wall conditions and processes, investigating droplet/aerosol removal (including sidewall losses), and conducting simplified experiments to isolate specific processes contributing to model divergence and reduce model uncertainties. 

Abstract Water vapor supersaturation in clouds is a random variable that drives activation and growth of cloud droplets. The Pi Convection–Cloud Chamber generates a turbulent cloud with a microphysical steady state that can be varied from clean to polluted by adjusting the aerosol injection rate. The supersaturation distribution and its moments, e.g., mean and variance, are investigated for varying cloud microphysical conditions. High-speed and collocated Eulerian measurements of temperature and water vapor concentration are combined to obtain the temporally resolved supersaturation distribution. This allows quantification of the contributions of variances and covariances between water vapor and temperature. Results are consistent with expectations for a convection chamber, with strong correlation between water vapor and temperature; departures from ideal behavior can be explained as resulting from dry regions on the warm boundary, analogous to entrainment. The saturation ratio distribution is measured under conditions that show monotonic increase of liquid water content and decrease of mean droplet diameter with increasing aerosol injection rate. The change in liquid water content is proportional to the change in water vapor concentration between no-cloud and cloudy conditions. Variability in the supersaturation remains even after cloud droplets are formed, and no significant buffering is observed. Results are interpreted in terms of a cloud microphysical Damköhler number (Da), under conditions corresponding to, i.e., the slow-microphysics regime. This implies that clouds with very clean regions, such thatis satisfied, will experience supersaturation fluctuations without them being buffered by cloud droplet growth. Significance StatementThe saturation ratio (humidity) in clouds controls the growth rate and formation of cloud droplets. When air in a turbulent cloud mixes, the humidity varies in space and time throughout the cloud. This is important because it means cloud droplets experience different growth histories, thereby resulting in broader size distributions. It is often assumed that growth and evaporation of cloud droplets buffers out some of the humidity variations. Measuring these variations has been difficult, especially in the field. The purpose of this study is to measure the saturation ratio distribution in clouds with a range of conditions. We measure the in-cloud saturation ratio using a convection cloud chamber with clean to polluted cloud properties. We found in clouds with low concentrations of droplets that the variations in the saturation ratio are not suppressed.