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The climate effects of atmospheric aerosol particles serving as cloud condensation nuclei (CCN) depend on chemical composition and hygroscopicity, which are highly variable on spatial and temporal scales. Here we present global CCN measurements, covering diverse environments from pristine to highly polluted conditions. We show that the effective aerosol hygroscopicity, κ, can be derived accurately from the fine aerosol mass fractions of organic particulate matter (ϵorg) and inorganic ions (ϵinorg) through a linear combination, κ = ϵorg ⋅ κorg + ϵinorg ⋅ κinorg. In spite of the chemical complexity of organic matter, its hygroscopicity is well captured and represented by a global average value of κorg = 0.12 ± 0.02 with κinorg = 0.63 ± 0.01 as the corresponding value for inorganic ions. By showing that the sensitivity of global climate forcing to changes in κorg and κinorg is small, we constrain a critically important aspect of global climate modelling.

General circulation models (GCMs), unlike other lines of evidence, indicate that anthropogenic aerosols cause a global-mean increase in cloud liquid water path (L) and thus a negative adjustment to radiative forcing of the climate by aerosol–cloud interactions. In part 1 of this series of papers, we showed that this is true even in models that reproduce the negative correlation observed in present-day internal variability in L and cloud droplet number concentration (Nd). We studied several possible confounding mechanisms that could explain the noncausal cloud–aerosol correlations in GCMs and that possibly contaminate observational estimates of radiative adjustments. Here, we perform single-column and full-atmosphere GCM experiments to investigate the causal model-physics mechanisms underlying the model radiative adjustment estimate. We find that both aerosol–cloud interaction mechanisms thought to be operating in real clouds – precipitation suppression and entrainment evaporation enhancement – are active in GCMs and behave qualitatively in agreement with physical process understanding. However, the modeled entrainment enhancement has a negligible global-mean effect. This raises the question of whether the GCM estimate is incorrect due to parametric or base-state representation errors or whether the process understanding gleaned from a limited set of canonical cloud cases is insufficiently representative of the diversity of clouds in the real climate. Regardless, even at limited resolution, the GCM physics appears able to parameterize the small-scale microphysics–turbulence interplay responsible for the entrainment enhancement mechanism. We suggest ways to resolve tension between current and future (storm-resolving) global modeling systems and other lines of evidence in synthesis climate projections. [ABSTRACT FROM AUTHOR]

A technique is presented that uses attenuated backscatter profiles from the CALIOP satellite lidar to estimate cloud base heights of lower-troposphere liquid clouds (cloud base height below approximately 3 km). Even when clouds are thick enough to attenuate the lidar beam (optical thickness τ≥5), the technique provides cloud base heights by treating the cloud base height of nearby thinner clouds as representative of the surrounding cloud field. Using ground-based ceilometer data, uncertainty estimates for the cloud base height product at retrieval resolution are derived as a function of various properties of the CALIOP lidar profiles. Evaluation of the predicted cloud base heights and their predicted uncertainty using a second statistically independent ceilometer dataset shows that cloud base heights and uncertainties are biased by less than 10 %. Geographic distributions of cloud base height and its uncertainty are presented. In some regions, the uncertainty is found to be substantially smaller than the 480m uncertainty assumed in the A-Train surface downwelling longwave estimate, potentially permitting the most uncertain of the radiative fluxes in the climate system to be better constrained.

Heterogeneous radiative forcing in mid-latitudes, such as that exerted by aerosols, has been found to affect the Arctic climate, though the mechanisms remain debated. In this study, we leverage deep learning (DL) techniques to explore the complex response of the Arctic climate system to local radiative forcing over Europe. We conducted sensitivity experiments using the Max Planck Institute Earth System Model (MPI-ESM1.2) coupled with atmosphere–ocean–land-surface components. Large-scale circulation patterns can mediate the impact of the forcing on Arctic climate dynamics. We employed a DL-based clustering approach to classify large-scale atmospheric circulation patterns. To enhance the analysis of how these patterns impact the Arctic climate, the poleward moist static energy transport (PMSET) associated with the atmospheric circulation patterns was incorporated as an additional similarity metric in the clustering process. Furthermore, we developed a novel method to analyze the circulation patterns' contributions to various climatic parameter anomalies. Our findings indicate that the negative radiative forcing over Europe alters existing circulation patterns and their occurrence frequency without introducing new ones. Specifically, our analysis revealed that while the regional radiative forcing alters the occurrence frequencies of the circulation patterns, these changes are not the primary drivers of the forcing's impact on the Arctic parameters. Instead, it is the shifts in the mean spatial characteristics of the atmospheric circulation patterns, induced by the forcing, that predominantly determine the effects on the Arctic climate. Our methodology facilitates the uncovering of complex, nonlinear interactions within the climate system, capturing nuances that are often obscured in broader seasonal anomaly analyses. This approach enables a deeper understanding of the dynamics driving observed climatic anomalies and their links to specific atmospheric circulation patterns. [ABSTRACT FROM AUTHOR]

Clouds are a crucial regulator in the Earth's energy budget through their radiative properties, both at the top of the atmosphere and at the surface; hence, determining key factors like their vertical extent is of essential interest. While the cloud top height is commonly retrieved by satellites, the cloud base height is difficult to estimate from satellite remote sensing data. Here, we present a novel method called ORABase (Ordinal Regression Auto-encoding of cloud Base), leveraging spatially resolved cloud properties from the Moderate Resolution Imaging Spectroradiometer (MODIS) instrument to retrieve the cloud base height over marine areas. A machine learning model is built with two components to facilitate the cloud base height retrieval: the first component is an auto-encoder designed to learn a representation of the data cubes of cloud properties and to reduce their dimensionality. The second component is developed for predicting the cloud base using ground-based ceilometer observations from the lower-dimensional encodings generated by the aforementioned auto-encoder. The method is then evaluated based on a collection of collocated surface ceilometer observations and retrievals from the CALIOP satellite lidar. The statistical model performs similarly on both datasets and performs notably well on the test set of ceilometer cloud bases, where it exhibits accurate predictions, particularly for lower cloud bases, and a narrow distribution of the absolute error, namely 379 and 328 m for the mean absolute error and the standard deviation of the absolute error, respectively. Furthermore, cloud base height predictions are generated for an entire year over the ocean, and global mean aggregates are also presented, providing insights into global cloud base height distributions and offering a valuable dataset for extensive studies requiring global cloud base height retrievals. The global cloud base height dataset and the presented models constituting ORABase are available from Zenodo (Lenhardt et al., 2024). [ABSTRACT FROM AUTHOR]

Over the past few decades, the geographical distribution of emissions of substances that alter the atmospheric energy balance has changed due to economic growth and air pollution regulations. Here, we show the resulting changes to aerosol and ozone abundances and their radiative forcing using recently updated emission data for the period 1990-2015, as simulated by seven global atmospheric composition models. The models broadly reproduce large-scale changes in surface aerosol and ozone based on observations (e.g.-1 to-3%yr-1 in aerosols over the USA and Europe). The global mean radiative forcing due to ozone and aerosol changes over the 1990-2015 period increased by +0.17±0.08Wm-2, with approximately one-third due to ozone. This increase is more strongly positive than that reported in IPCC AR5. The main reasons for the increased positive radiative forcing of aerosols over this period are the substantial reduction of global mean SO2 emissions, which is stronger in the new emission inventory compared to that used in the IPCC analysis, and higher black carbon emissions.

In this study we explore aerosol–cloud interactions in liquid-phase clouds over eastern China (EC) and its adjacent ocean (ECO) using the WRF-Chem–SBM model with four-dimensional assimilation. The results show that our simulations and analyses based on each vertical layer provide a more detailed representation of the aerosol–cloud relationship compared to the column-based analyses which have been widely conducted previously. For aerosol activation, cloud droplet number concentration (Nd) generally increases with aerosol number concentration (Naero) at low Naero and decreases with Naero at high Naero. The main difference between EC and ECO is that Nd increases faster in ECO than EC at low Naero due to abundant water vapor, whereas at high Naero , when aerosol activation in ECO is suppressed, Nd in EC shows significant fluctuation due to strong surface effects (longwave radiation cooling and terrain uplift) and intense updrafts. Cloud liquid water content (CLWC) increases with Nd , but the increase rate gradually slows down for precipitating clouds, while CLWC increases and then decreases in non-precipitating clouds. Higher Nd and CLWC can be found in EC than in ECO, and the transition-point Nd value at which CLWC in non-precipitating clouds changes from increasing to decreasing is also higher in EC. Aerosol activation is strongest at moderate Naero , but CLWC increases relatively fast at low Naero. ECO cloud processes are more limited by cooling and humidification, whereas strong and diverse surface and atmospheric processes in EC allow intense cloud processes to occur under significant warming or drying conditions. [ABSTRACT FROM AUTHOR]

Surface air temperature (SAT) is a key indicator of climate change. Variations in cloud cover affect SAT by interacting with radiation. During daytime, clouds tend to cool the surface by blocking sunlight, while nighttime clouds warm the surface by trapping longwave radiation. Here, we show that, on the global scale, cloud cover, particularly low-level cloudiness, exhibits diurnally asymmetric trends in a warming climate. Cloud fraction on average decreases more during the day than at night. Climate models indicate that the diurnally asymmetric cloud cover variation is mainly driven by trends in the lower tropospheric stability and is largely attributed to the increasing greenhouse gases rather than natural variability. This asymmetry, therefore, turns out to be an amplifier of surface warming, by both decreasing the daytime cloud shortwave albedo effect and increasing the nighttime cloud longwave greenhouse effect. [ABSTRACT FROM AUTHOR]

General circulation models' (GCMs) estimates of the liquid water path adjustment to anthropogenic aerosol emissions differ in sign from other lines of evidence. This reduces confidence in estimates of the effective radiative forcing of the climate by aerosol–cloud interactions (ERFaci). The discrepancy is thought to stem in part from GCMs' inability to represent the turbulence–microphysics interactions in cloud-top entrainment, a mechanism that leads to a reduction in liquid water in response to an anthropogenic increase in aerosols. In the real atmosphere, enhanced cloud-top entrainment is thought to be the dominant adjustment mechanism for liquid water path, weakening the overall ERFaci. We show that the latest generation of GCMs includes models that produce a negative correlation between the present-day cloud droplet number and liquid water path, a key piece of observational evidence supporting liquid water path reduction by anthropogenic aerosols and one that earlier-generation GCMs could not reproduce. However, even in GCMs with this negative correlation, the increase in anthropogenic aerosols from preindustrial to present-day values still leads to an increase in the simulated liquid water path due to the parameterized precipitation suppression mechanism. This adds to the evidence that correlations in the present-day climate are not necessarily causal. We investigate sources of confounding to explain the noncausal correlation between liquid water path and droplet number. These results are a reminder that assessments of climate parameters based on multiple lines of evidence must carefully consider the complementary strengths of different lines when the lines disagree. [ABSTRACT FROM AUTHOR]

Author(s): Velle Toll [sup.1] [sup.2] , Matthew Christensen [sup.3] , Johannes Quaas [sup.4] , Nicolas Bellouin [sup.1] Author Affiliations: (1) Department of Meteorology, University of Reading, Reading, UK (2) Institute [...], The cooling of the Earth's climate through the effects of anthropogenic aerosols on clouds offsets an unknown fraction of greenhouse gas warming. An increase in the amount of water inside liquid-phase clouds induced by aerosols, through the suppression of rain formation, has been postulated to lead to substantial cooling, which would imply that the Earth's surface temperature is highly sensitive to anthropogenic forcing. Here we provide direct observational evidence that, instead of a strong increase, aerosols cause a relatively weak average decrease in the amount of water in liquid-phase clouds compared with unpolluted clouds. Measurements of polluted clouds downwind of various anthropogenic sources--such as oil refineries, smelters, coal-fired power plants, cities, wildfires and ships--reveal that aerosol-induced cloud-water increases, caused by suppressed rain formation, and decreases, caused by enhanced evaporation of cloud water, partially cancel each other out. We estimate that the observed decrease in cloud water offsets 23% of the global climate-cooling effect caused by aerosol-induced increases in the concentration of cloud droplets. These findings invalidate the hypothesis that increases in cloud water cause a substantial climate cooling effect and translate into reduced uncertainty in projections of future climate. Satellite data for cloud tracks downwind of major pollution sources show a relatively small global average decrease in cloud water caused by anthropogenic aerosols, invalidating claims that aerosol-induced effects contribute substantially to climate cooling.