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Weather and climate models are challenged by uncertainties and biases in simulating Southern Ocean (SO) radiative fluxes that trace to a poor understanding of cloud, aerosol, precipitation, and radiative processes, and their interactions. Projects between 2016 and 2018 used in situ probes, radar, lidar, and other instruments to make comprehensive measurements of thermodynamics, surface radiation, cloud, precipitation, aerosol, cloud condensation nuclei (CCN), and ice nucleating particles over the SO cold waters, and in ubiquitous liquid and mixed-phase clouds common to this pristine environment. Data including soundings were collected from the NSF–NCAR G-V aircraft flying north–south gradients south of Tasmania, at Macquarie Island, and on the R/V Investigator and RSV Aurora Australis. Synergistically these data characterize boundary layer and free troposphere environmental properties, and represent the most comprehensive data of this type available south of the oceanic polar front, in the cold sector of SO cyclones, and across seasons. Results show largely pristine environments with numerous small and few large aerosols above cloud, suggesting new particle formation and limited long-range transport from continents, high variability in CCN and cloud droplet concentrations, and ubiquitous supercooled water in thin, multilayered clouds, often with small-scale generating cells near cloud top. These observations demonstrate how cloud properties depend on aerosols while highlighting the importance of dynamics and turbulence that likely drive heterogeneity of cloud phase. Satellite retrievals confirmed low clouds were responsible for radiation biases. The combination of models and observations is examining how aerosols and meteorology couple to control SO water and energy budgets.

The aerosol–cloud–precipitation interactions within the cloud-topped marine boundary layer (MBL) are examined using aircraft in situ measurements from Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) and Southern Ocean Clouds, Radiation, Aerosol Transport Experimental Study (SOCRATES) field campaigns. SOCRATES clouds exhibit a larger number concentration and smaller cloud droplet effective radius (148.3 cm−3 and 8.0 µm) compared to ACE-ENA summertime (89.4 cm−3 and 9.0 µm) and wintertime clouds (70.6 cm−3 and 9.8 µm). The ACE-ENA clouds, especially during the winter, feature stronger drizzle formation via droplet growth through enhanced collision–coalescence that is attributed to a relatively cleaner environment and deeper cloud layer. Furthermore, the aerosol–cloud interaction (ACI) indices from the two aircraft field campaigns exhibit distinct sensitivities, indicating different cloud microphysical responses to aerosols. The ACE-ENA winter season features relatively fewer aerosols, which are more likely activated into cloud droplets under the conditions of sufficient water vapor availability and strong turbulence. The enriched aerosol loading during ACE-ENA summer and SOCRATES generally leads to smaller cloud droplets competing for the limited water vapor and exhibiting a stronger ACI. Notably, the precipitation susceptibilities are stronger during the ACE-ENA than during the SOCRATES campaigns. The in-cloud drizzle behavior significantly alters sub-cloud cloud condensation nuclei (CCN) budgets through the coalescence-scavenging effect and, in turn, impacts the ACI assessments. The results of this study can enhance understanding and aid in future model simulation and assessment of the aerosol–cloud interaction.

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.

The new Energy Exascale Earth System Model Version 1 (E3SMv1) developed for the U.S. Department of Energy has significant new treatments of aerosols and light‐absorbing snow impurities as well as their interactions with clouds and radiation. This study describes seven sets of new aerosol‐related treatments (involving emissions, new particle formation, aerosol transport, wet scavenging and resuspension, and snow radiative transfer) and examines how they affect global aerosols and radiative forcing in E3SMv1. Altogether, they give a reduced total aerosol radiative forcing (−1.6 W/m2) and sensitivity in cloud liquid water to aerosols, but an increased sensitivity in cloud droplet size to aerosols. A new approach for H2SO4 production and loss largely reduces a low bias in small particles concentrations and leads to substantial increases in cloud condensation nuclei concentrations and cloud radiative cooling. Emitting secondary organic aerosol precursor gases from elevated sources increases the column burden of secondary organic aerosol, contributing substantially to global clear‐sky aerosol radiative cooling (−0.15 out of −0.5 W/m2). A new treatment of aerosol resuspension from evaporating precipitation, developed to remedy two shortcomings of the original treatment, produces a modest reduction in aerosols and cloud droplets; its impact depends strongly on the model physics and is much stronger in E3SM Version 0. New treatments of the mixing state and optical properties of snow impurities and snow grains introduce a positive present‐day shortwave radiative forcing (0.26 W/m2), but changes in aerosol transport and wet removal processes also affect the concentration and radiative forcing of light‐absorbing impurities in snow/ice. Plain Language Summary Aerosol and aerosol‐cloud interactions continue to be a major uncertainty in Earth system models, impeding their ability to reproduce the observed historical warming and to project changes in global climate and water cycle. The U.S. DOE Energy Exascale Earth System Model version 1 (E3SMv1), a state‐of‐the‐science Earth system model, was developed to use exascale computing to address the grand challenge of actionable predictions of variability and change in the Earth system critical to the energy sector. It has been publicly released with new treatments in many aspects, including substantial modifications to the physical treatments of aerosols in the atmosphere and light‐absorbing impurities in snow/ice, aimed at reducing some known biases or correcting model deficiencies in representing aerosols, their life cycle, and their impacts in various components of the Earth system. Compared to its predecessors (without the new treatments) and observations, E3SMv1 shows improvements in characterizing global distributions of aerosols and their radiative effects. We conduct sensitivity experiments to understand the impact of individual changes and provide guidance for future development of E3SM and other Earth system models. Key Points A description and assessment of new aerosol treatments in the Energy Exascale Earth System Model Version 1 (E3SMv1) is provided Contributions to the total aerosol‐related radiative forcing by individual new treatments and different processes are quantified Some of the new treatments are found to depend on model physics and require further improvement for E3SM or other Earth system models

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.

The Weather Research and Forecasting (WRF) Model coupled with a spectral bin microphysics (SBM) scheme is used to investigate aerosol effects on cloud microphysics and precipitation over the Indian peninsular region. The main emphasis of the study is in comparing simulated cloud microphysical structure with in situ aircraft observations from the Cloud Aerosol Interaction and Precipitation Enhancement Experiment (CAIPEEX). Aerosol–cloud interaction over the rain-shadow region is investigated with observed and simulated size distribution spectra of cloud droplets and ice particles in monsoon clouds. It is shown that size distributions as well as other microphysical characteristics obtained from simulations such as liquid water content, cloud droplet effective radius, cloud droplet number concentration, and thermodynamic parameters are in good agreement with the observations. It is seen that in clouds with high cloud condensation nuclei (CCN) concentrations, snow and graupel size distribution spectra were broader compared to clouds with low concentrations of CCN, mainly because of enhanced riming in the presence of a large number of droplets with a diameter of 10–30 μm. The Hallett–Mossop ice multiplication process is illustrated to have an impact on snow and graupel mass. The changes in CCN concentrations have a strong effect on cloud properties over the domain, amounts of cloud water, and the glaciation of the clouds, but the effects on surface precipitation are small when averaged over a large area. Overall enhancement of cold-phase cloud processes in the high-CCN case contributed to slight enhancement (5%) in domain-averaged surface precipitation.

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.

For the first time, a closure study of the relationship between the ice-nucleating particle concentration (INP; INPC) and ice crystal number concentration (ICNC) in altocumulus and cirrus layers, solely based on ground-based active remote sensing, is presented. Such aerosol–cloud closure experiments are required (a) to better understand aerosol–cloud interaction in the case of mixed-phase clouds, (b) to explore to what extent heterogeneous ice nucleation can contribute to cirrus formation, which is usually controlled by homogeneous freezing, and (c) to check the usefulness of available INPC parameterization schemes, applied to lidar profiles of aerosol optical and microphysical properties up to the tropopause level. The INPC–ICNC closure studies were conducted in Cyprus (Limassol and Nicosia) during a 6-week field campaign in March–April 2015 and during the 17-month CyCARE (Cyprus Clouds Aerosol and Rain Experiment) campaign. The focus was on altocumulus and cirrus layers which developed in pronounced Saharan dust layers at heights from 5 to 11 km. As a highlight, a long-lasting cirrus event was studied which was linked to the development of a very strong dust-infused baroclinic storm (DIBS) over Algeria. The DIBS was associated with strong convective cloud development and lifted large amounts of Saharan dust into the upper troposphere, where the dust influenced the evolution of an unusually large anvil cirrus shield and the subsequent transformation into an cirrus uncinus cloud system extending from the eastern Mediterranean to central Asia, and thus over more than 3500 km. Cloud top temperatures of the three discussed closure study cases ranged from −20 to −57 ∘C. The INPC was estimated from polarization/Raman lidar observations in combination with published INPC parameterization schemes, whereas the ICNC was retrieved from combined Doppler lidar, aerosol lidar, and cloud radar observations of the terminal velocity of falling ice crystals, radar reflectivity, and lidar backscatter in combination with the modeling of backscattering at the 532 and 8.5 mm wavelengths. A good-to-acceptable agreement between INPC (observed before and after the occurrence of the cloud layer under investigation) and ICNC values was found in the discussed three proof-of-concept closure experiments. In these case studies, INPC and ICNC values matched within an order of magnitude (i.e., within the uncertainty ranges of the INPC and ICNC estimates), and they ranged from 0.1 to 10 L−1 in the altocumulus layers and 1 to 50 L−1 in the cirrus layers observed between 8 and 11 km height. The successful closure experiments corroborate the important role of heterogeneous ice nucleation in atmospheric ice formation processes when mineral dust is present. The observed long-lasting cirrus event could be fully explained by the presence of dust, i.e., without the need for homogeneous ice nucleation processes.

Relative dispersion (ε), as a parameter characterizing droplet spectral shape, exerts a considerable impact on cloud radiation and precipitation processes, and its accurate parameterization is urgently needed in models. Current ε parameterizations, which are based on droplet number concentration or simply set as constants, are inadequate to satisfy the demand. This study shows, utilizing in‐situ cloud and fog observations from five underlying surface regions (urban, suburban, mountainous, coastal and rainforest) of China, that ε uniformly and stably manifests as initially increasing then decreasing as volume‐mean diameter increases across these regions. Based on this relationship, a ε parameterization is established, which exhibits improved predictive capabilities in evaluating both cloud albedo effect and cloud lifetime effect. The parameterization is expected to enhance cloud simulation accuracy and minimize discrepancy between observed and simulated cloud radiation and precipitation, particularly for weather and climate models that commonly use the double‐moment cloud microphysical schemes. Plain Language Summary Clouds play a crucial role in the Earth's weather and climate. One key factor in understanding cloud behavior is the width of cloud droplet size distribution, quantified by relative dispersion. Accurately representing relative dispersion in weather and climate models is essential, yet current methods are often overly simplistic. Many models either rely on fixed values or use empirical monotonic equations based solely on droplet number concentration. However, the relationship between relative dispersion and droplet number concentration varies significantly across regions and can even be contradictory. In this study, we analyzed cloud and fog observations from five different regions, encompassing urban, suburban, mountainous, coastal, and rainforest environments. Our analysis revealed a consistent pattern: relative dispersion first increases and then decreases as the volume‐mean droplet diameter grows. Based on this insight, we developed a new method to predict relative dispersion. This approach has the potential to improve the accuracy of estimating cloud albedo and lifetime effects, enhancing the representation of aerosol‐cloud interactions in weather and climate models. Key Points Correlation between droplet spectral dispersion and volume‐mean diameter remains consistent across different regions Compared to previous dispersion parameterizations, the parameterization with volume‐mean diameter provides better predictions for dispersion The dispersion parameterization with volume‐mean diameter could reduce the uncertainty in simulating aerosol indirect effects

Changes in land cover and aerosols resulting from urbanization may impact convective clouds and precipitation. Here we investigate how Houston urbanization can modify sea-breeze-induced convective cloud and precipitation through the urban land effect and anthropogenic aerosol effect. The simulations are carried out with the Chemistry version of the Weather Research and Forecasting model (WRF-Chem), which is coupled with spectral-bin microphysics (SBM) and the multilayer urban model with a building energy model (BEM-BEP). We find that Houston urbanization (the joint effect of both urban land and anthropogenic aerosols) notably enhances storm intensity (by ∼ 75 % in maximum vertical velocity) and precipitation intensity (up to 45 %), with the anthropogenic aerosol effect more significant than the urban land effect. Urban land effect modifies convective evolution: speed up the transition from the warm cloud to mixed-phase cloud, thus initiating surface rain earlier but slowing down the convective cell dissipation, all of which result from urban heating-induced stronger sea-breeze circulation. The anthropogenic aerosol effect becomes evident after the cloud evolves into the mixed-phase cloud, accelerating the development of storm from the mixed-phase cloud to deep cloud by ∼ 40 min. Through aerosol–cloud interaction (ACI), aerosols boost convective intensity and precipitation mainly by activating numerous ultrafine particles at the mixed-phase and deep cloud stages. This work shows the importance of considering both the urban land and anthropogenic aerosol effects for understanding urbanization effects on convective clouds and precipitation.