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Quantifying the aerosol/cloud-mediated radiative effect at a global scale requires simultaneous satellite retrievals of cloud condensation nuclei (CCN) concentrations and cloud base updraft velocities (Wb ). Hitherto, the inability to do so has been a major cause of high uncertainty regarding anthropogenic aerosol/cloud-mediated radiative forcing. This can be addressed by the emerging capability of estimating CCN and Wb of boundary layer convective clouds from an operational polar orbiting weather satellite. Our methodology uses such clouds as an effective analog for CCN chambers. The cloud base supersaturation (S) is determined by Wb and the satellite-retrieved cloud base drop concentrations (Ndb ), which is the same as CCN(S). Validation against ground-based CCN instruments at Oklahoma, at Manaus, and onboard a ship in the northeast Pacific showed a retrieval accuracy of ±25% to ±30% for individual satellite overpasses. The methodology is presently limited to boundary layer not raining convective clouds of at least 1 km depth that are not obscured by upper layer clouds, including semitransparent cirrus. The limitation for small solar backscattering angles of <25° restricts the satellite coverage to ∼25% of the world area in a single day.

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

Anthropogenic aerosols (AA) can affect cloud and precipitation through aerosol–radiation interaction (ARI) and aerosol–cloud interaction (ACI). Over the past few decades, anthropogenic aerosol emissions have exhibited remarkable changes in the magnitude and in spatial pattern. The most significant changes are the increased emissions over both South Asia and East Asia. In this study, the atmospheric component of a state-of-the-art climate model that includes eight species of tropospheric aerosols, coupled to a multi-level mixed-layer ocean model, has been used to investigate the impacts of Asian anthropogenic aerosol precursor emission changes from 1970s to 2000s on large scale circulation and precipitation in boreal summer over East Asia. Results reveal significant changes in circulation and clouds over East Asia and over the tropical and western North Pacific (WNP). Increased Asian AA emissions lead to anomalous cyclonic circulation over the Maritime continent (MC) and anomalous anticyclonic circulation over the WNP, resulting in anomalous moisture transport convergence over the MC and therefore increased precipitation. They also lead to anomalous moisture flux divergence over both the WNP and large land areas of East Asia, especially over northern China, and therefore decreased precipitation there. These large scale circulation anomalies over the adjacent oceans are related to aerosol change induced ocean feedbacks, predominantly through ACI. It is the slow responses over the adjacent oceans (e.g., SST changes) through coupled atmosphere–ocean interaction in pre-monsoon seasons and summer that shape the changes of the East Asian summer monsoon and local precipitation. The results in this study suggest that increased Asian AA emissions from 1970s to 2000s may have played an important role for the observed southward shift of the Pacific intertropical convergence zone and precipitation belt, weakening of East Asian summer monsoon and reduced precipitation over northern China in East Asia during the latter half of the twentieth century.

Recent observations show that dust emitted within the Arctic (Arctic dust) has a remarkably high ice nucleating ability, especially between −20°C and −5°C, but its impacts on the number concentrations of ice nucleating particles (INPs) and radiative balance in the Arctic are not well understood. Here we incorporate an observation‐based ice‐nucleation parameterization indicating the high ice nucleating ability of Arctic dust into a global aerosol‐climate model. A simulation using this parameterization better reproduces INP observations in the Arctic and estimates >100 times higher dust INP number concentrations with ∼100% contribution from Arctic dust in the Arctic lower troposphere (>60°N and >700 hPa) during summer and fall (June–November) than a simulation applying a standard ice‐nucleation parameterization suitable for desert dust to Arctic dust. Our results demonstrate the importance of considering an ice‐nucleation parameterization suitable for Arctic dust when simulating INPs and their effects on aerosol‐cloud interactions in the Arctic. Plain Language Summary Dust is an important aerosol type acting as “ice nucleating particles,” which initiate the formation of ice crystals within mixed‐phase clouds (consisting of both supercooled water droplets and ice crystals) and influence the cloud lifetime and distribution. Recent observations show that dust is emitted from ice‐ and vegetation‐free areas in the Arctic region (hereafter Arctic dust), which has a remarkably high ice nucleating ability, compared with desert dust such as Asian dust and Saharan dust, because of the presence of certain organic matter. However, the impacts of Arctic dust with high ice nucleating ability on ice nucleating particles and mixed‐phase clouds in the Arctic are unknown. In this study, we investigate the importance of Arctic dust with high ice nucleating ability for ice nucleating particles in the Arctic using a global aerosol‐climate model. Our simulation results show that Arctic dust accounts for almost all dust ice nucleating particles in the Arctic lower troposphere (>60°N and about 0–3 km) during summer and fall (June–November). This study demonstrates the importance of considering the high ice nucleating ability of Arctic dust when simulating ice nucleating particles and their impacts on mixed‐phase clouds and radiative balance in the Arctic. Key Points Arctic dust, emitted within the Arctic, accounts for most of dust ice nucleating particles in the Arctic lower troposphere in summer to fall Importance of Arctic dust as ice nucleating particles in the Arctic strongly depends on its high ice nucleating ability at high temperatures Considering an ice‐nucleation parameterization suitable for Arctic dust is crucial for aerosol‐cloud‐climate simulations in the Arctic

Aerosol-cloud interactions (ACI) in warm clouds are the primary source of uncertainty in effective radiative forcing (ERF) during the historical period and, by extension, inferred climate sensitivity. The ERF due to ACI (ERFaci) is composed of the radiative forcing due to changes in cloud microphysics and cloud adjustments to microphysics. Here, we examine the processes that drive ERFaci using a perturbed parameter ensemble (PPE) hosted in CAM6. Observational constraints on the PPE result in substantial constraints in the response of cloud microphysics and macrophysics to anthropogenic aerosol, but only minimal constraint on ERFaci. Examination of cloud and radiation processes in the PPE reveal buffering of ERFaci by the interaction of precipitation efficiency and radiative susceptibility.

The influence of entrainment, a key process characterized by the entrainment rate in cumulus parameterization, on aerosol‐cloud interactions has been widely recognized. However, despite qualitative links established between entrainment and aerosol loading, a quantitative relationship based on observational evidence remains elusive. This study utilizes aircraft observations of cumulus clouds during two field campaigns to determine the quantitative relationship between entrainment rate and aerosol loading. In both campaigns, the entrainment rate is negatively correlated with aerosol loading. It is speculated that increased aerosol loading enhances cloud edge droplet evaporation, which leads to increased buoyancy and vertical velocity within the cloud, thereby reducing the entrainment rate. Further analysis shows that the response of entrainment rate to aerosol perturbations is more significant in smaller cumulus clouds with weak buoyancy and less pronounced under opposite conditions. These findings shed new light on improving the description of aerosol‐cloud interactions in cumulus parameterizations. Plain Language Summary Clouds play a crucial role in regulating Earth's climate, and understanding how they form and evolve is important for accurate weather and climate predictions. One key process affecting cloud development is entrainment, where drier air from outside the cloud mixes into the cloud, influencing its growth. Scientists know that aerosols can impact entrainment, but the exact relationship hasn't been clear. This study uses observations from research aircraft flown through cumulus clouds to quantify the relationship between entrainment and aerosol. The results show that aerosol concentration is negatively correlated with entrainment rate, meaning less dry air mixes into the cloud. We speculate that this happens because the increased aerosols enhance the evaporation of cloud droplets at the cloud edges, making the cloud more buoyant and less likely to mix with the surrounding air. Interestingly, this decline in entrainment rate to aerosol is stronger in smaller and weaker clouds. These findings provide valuable insights into how aerosols influence cloud development and can help improve the representation of aerosol‐cloud interactions in climate models, leading to more accurate climate projections. Key Points The relationship between cumulus entrainment rate and aerosol loading is quantified based on observation for the first time The plausible physical mechanism linking entrainment rate to aerosol loading has been elucidated A steeper decline in entrainment rate with increasing aerosol loading is observed in small and weakly buoyant cumulus clouds

Aerosol–cloud interactions present a large source of uncertainties in atmospheric and climate models. One of the main challenges to simulate ice clouds is to reproduce the right ice nucleating particle concentration. In this study, we derive a parameterization for immersion freezing according to the classical nucleation theory. Our objective was to constrain this parameterization with observations taken over the Canadian Arctic during the Amundsen summer 2014 and 2016 campaigns. We found a linear dependence of contact angle and temperature. Using this approach, we were able to reproduce the scatter in ice nucleated particle concentrations within a factor 5 of observed values with a small negative bias. This parameterization would be easy to implement in climate and atmospheric models, but its representativeness has to first be validated against other datasets.

By examining the historical temperature record during the industrial era, we can infer the climate's sensitivity to radiative perturbations, given knowledge of historical forcings. Energy conservation enforces a negative correlation between the climate feedback and historical forcing for a given change in global‐mean temperature. Here, we examine the negative correlation between the radiative forcing due to aerosol‐cloud interactions and the shortwave cloud feedback to warming that appears in a perturbed parameter ensemble (PPE). The PPE is not tuned to match the historical record, yet a negative correlation emerges over the extratropics due to the combined effects of liquid cloud precipitation efficiency and radiative saturation in the shortwave. Using an energy balance model, we argue that these processes combine to push Earth System Models to yield a temperature record in keeping with observations, but also limit our ability to constrain future warming posterior with the temperature record.

Atmospheric aerosols often contain surface‐active organics, which reduce surface tension and enhance cloud droplets activation. This effect is often neglected in the application of Köhler theory where a constant surface tension equivalent to pure water is assumed. Using a cloud parcel model, we evaluated the impact of four representative surface‐active organics, humic‐like substances (HULIS), sodium dodecyl sulfate (SDS), cis‐pinonic acid, and dicarboxylic acids, on cloud condensation nuclei (CCN) activation under varied atmospheric conditions. Our results indicate that HULIS significantly enhance CCN activation, particularly at high aerosol concentrations, low updraft velocities, and small particle sizes. SDS, cis‐pinonic acid, and dicarboxylic acids also increase activation but to a lesser degree. The surface activity of HULIS has a stronger influence on CCN activation than its hygroscopicity, with particle size being the most sensitive parameter. This study emphasizes the need to incorporate surface‐active organics into climate models to improve the prediction of aerosol‐cloud interactions.

The interaction between aerosols and clouds is one of the major uncertainties in past climate change, affecting the accuracy of future climate projections. Ship tracks, trails left in clouds through the addition of aerosol in the ship exhaust plume, have become a key observational tool for constraining aerosol‐cloud interactions. However, many expected tracks remain undetected, presenting a significant gap in current knowledge of aerosol forcing. Here we leverage a plume‐parcel model to simulate the impact of aerosol dispersion for 2,957 cases off California's coast on cloud droplet number concentration (CDNC) enhancements. Plume‐parcel models show a large sensitivity to updraft uncertainties, which are found to be a primary control on track formation. Using these plume‐parcel models, updraft values consistent with observed CDNC enhancements are recovered, suggesting that relying solely on cloud‐top radiative cooling may overestimate in‐cloud updrafts by around 50%, hence overstating the cloud sensitivity to aerosols. Plain Language Summary Here we investigate the interactions between aerosols and clouds and their impact on climate change. Ship tracks were used to study these interactions, and aerosol emissions from ships were modeled. It was shown that the increase in cloud droplets from ship aerosol was highly sensitive to the speed of the updraft in the clouds. A method was developed to fit the updraft to the observed cloud enhancements; the resultant updrafts were smaller than current estimates, suggesting that the clouds may be less sensitive to aerosols than previously thought. Key Points Using ship emission data, a plume‐parcel model was implemented to study aerosol availability and cloud sensitivity in ship track formation Cloud droplet number enhancements are very sensitive to uncertainties in the in‐cloud updraft The retrieved plume‐parcel‐based updrafts suggest that clouds may be less sensitive to aerosols than implied by other estimates