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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.

The Weather Research Forecasting (WRF) version 4.3 model is configured within a Lagrangian framework to quantify the impact of aerosols on evolving cloud fields. Kilometer-scale simulations utilizing meteorological boundary conditions are based on 10 case study days offering diverse meteorology during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA). Measurements from aircraft, the ground-based Atmosphere Radiation Measurement (ARM) site at Graciosa Island in the Azores, and A-Train and geostationary satellites are utilized for validation, demonstrating good agreement with the WRF-simulated cloud and aerosol properties. Higher aerosol concentration leads to suppressed drizzle and increased cloud water content in all case study days. These changes lead to larger radiative cooling rates at cloud top, enhanced vertical velocity variance, and increased vertical and horizontal wind speed near the base of the lower-tropospheric inversion. As a result, marine cloud cell area expands, narrowing the gap between shallow clouds and increasing cloud optical thickness, liquid water content, and the top-of-atmosphere outgoing shortwave flux. While similar aerosol effects are observed in lightly to non-raining clouds, they tend to be smaller by comparison. These simulations show a relationship between cloud cell area expansion and the radiative adjustments caused by liquid water path and cloud fraction changes. The adjustments are positive and scale as 74 % and 51 %, respectively, relative to the Twomey effect. While higher-resolution large-eddy simulations may provide improved representation of cloud-top mixing processes, these results emphasize the importance of addressing mesoscale cloud-state transitions in the quantification of aerosol radiative forcing that cannot be attained from traditional climate models.

Process-oriented observational constraints for the anthropogenic effective radiative forcing due to aerosol–cloud interactions (ERFaci) are highly desirable because the uncertainty associated with ERFaci poses a significant challenge to climate prediction. The contoured frequency by optical depth diagram (CFODD) analysis supports the evaluation of model representation of cloud liquid-to-rain conversion processes because the slope of a CFODD, generated from joint MODerate Resolution Imaging Spectroradiometer (MODIS)-CloudSat cloud retrievals, provides an estimate of cloud droplet collection efficiency in single-layer warm liquid clouds. Here, we present an updated CFODD analysis as an observational constraint on the ERFaci due to warm rain processes and apply it to the U.S. Department of Energy's Energy Exascale Earth System Model version 2 (E3SMv2). A series of sensitivity experiments shows that E3SMv2 droplet collection efficiencies and ERFaci are highly sensitive to autoconversion, i.e., the rate of mass transfer from cloud liquid to rain, yielding a strong correlation between the CFODD slope and the shortwave component of ERFaci (ERFaciSW; Pearson's R=-0.91). E3SMv2's CFODD slope (0.20 ± 0.04) is in agreement with observations (0.20 ± 0.03). The strong sensitivity of ERFaciSW to the CFODD slope provides a useful constraint on highly uncertain warm rain processes, whereby ERFaciSW, constrained by MODIS-CloudSat, is estimated by calculating the intercept of the linear association between the ERFaciSW and the CFODD slopes, using the MODIS-CloudSat CFODD slope as a reference.

Abstract Ships brighten low marine clouds from emissions of sulfur and aerosols, resulting in visible “ship tracks”. In 2020, new shipping regulations mandated an ∼80% reduction in the allowed fuel sulfur content. Recent observations indicate that visible ship tracks have decreased. Model simulations indicate that since 2020 shipping regulations have induced a net radiative forcing of +0.12 Wm−2. Analysis of recent temperature anomalies indicates Northern Hemisphere surface temperature anomalies in 2022–2023 are correlated with observed cloud radiative forcing and the cloud radiative forcing is spatially correlated with the simulated radiative forcing from the 2020 shipping emission changes. Shipping emissions changes could be accelerating global warming. To better constrain these estimates, better access to ship position data and understanding of ship aerosol emissions are needed. Understanding the risks and benefits of emissions reductions and the difficultly in robust attribution highlights the large uncertainty in attributing proposed deliberate climate intervention.

The impact of aerosol number concentration on cloud albedo is a persistent source of spread in global climate predictions due to multi-scale, interactive atmospheric processes that remain difficult to quantify. We use 5 years of geostationary satellite and surface retrievals at the US Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) eastern North Atlantic (ENA) site in the Azores to evaluate the representation of liquid cloud albedo susceptibility for overcast cloud scenes in the DOE Energy Exascale Earth System Model version 1 (E3SMv1) and provide possible reasons for model–observation discrepancies. The overall distribution of surface 0.2 % CCN concentration values is reasonably simulated, but simulated liquid water path (LWP) is lower than observed and layer mean droplet concentration (Nd) comparisons are highly variable depending on the Nd retrieval technique. E3SMv1's cloud albedo is greater than observed for given LWP and Nd values due to a lower cloud effective radius than observed. However, the simulated albedo response to Nd is suppressed due to a correlation between the solar zenith angle (SZA) and Nd created by the seasonal cycle that is not observed. Controlling for this effect by examining the cloud optical depth (COD) shows that E3SMv1's COD response to CCN concentration is greater than observed. For surface-based retrievals, this is only true after controlling for cloud adiabaticity because E3SMv1's adiabaticities are much lower than observed. Assuming a constant adiabaticity in surface retrievals as done in top-of-atmosphere (TOA) retrievals narrows the retrieved ln Nd distribution, which increases the cloud albedo sensitivity to ln Nd to match the TOA sensitivity. The greater sensitivity of COD to CCN is caused by a greater Twomey effect in which the sensitivity of Nd to CCN is greater than observed for TOA-retrieved Nd, and once model–observation cloud adiabaticity differences are removed, this is also true for surface-retrieved Nd. The LWP response to Nd in E3SMv1 is overall negative as observed. Despite reproducing the observed LWP–Nd relationship, observed clouds become much more adiabatic as Nd increases, while E3SMv1 clouds do not, associated with more heavily precipitating clouds that are partially but not completely caused by deeper clouds and weaker inversions in E3SMv1. These cloud property differences indicate that the negative LWP–Nd relationship is likely not caused by the same mechanisms in E3SMv1 and observations. The negative simulated LWP response also fails to mute the excessively strong Twomey effect, highlighting potentially important confounding factor effects that likely render the LWP–Nd relationship non-causal. Nd retrieval scales and assumptions, particularly related to cloud adiabaticity, contribute to substantial spreads in the model–observation comparisons, though enough consistency exists to suggest that aerosol activation, drizzle, and entrainment processes are critical areas to focus E3SMv1 development for improving the fidelity of aerosol–cloud interactions in E3SM.

Human aerosol emissions change cloud properties by providing additional cloud condensation nuclei. This increases cloud droplet numbers, which in turn affects other cloud properties like liquid-water content and ultimately cloud albedo. These adjustments are poorly constrained, making aerosol effects the most uncertain part of anthropogenic climate forcing. Here we show that cloud droplet number and water content react differently to changing emission amounts in shipping exhausts. We use information about ship positions and modeled emission amounts together with reanalysis winds and satellite retrievals of cloud properties. The analysis reveals that cloud droplet numbers respond linearly to emission amount over a large range (1–10 kg h−1) before the response saturates. Liquid water increases in raining clouds, and the anomalies are constant over the emission ranges observed. There is evidence that this independence of emissions is due to compensating effects under drier and more humid conditions, consistent with suppression of rain by enhanced aerosol. This has implications for our understanding of cloud processes and may improve the way clouds are represented in climate models, in particular by changing parameterizations of liquid-water responses to aerosol.

Automated methods for the detection and tracking of deep convective clouds in geostationary satellite imagery have a vital role in both the forecasting of severe storms and research into their behaviour. Studying the interactions and feedbacks between multiple deep convective clouds (DCC), however, poses a challenge for existing algorithms due to the necessary compromise between false detection and missed detection errors. We utilise an optical flow method to determine the motion of deep convective clouds in GOES-16 ABI imagery in order to construct a semi-Lagrangian framework for the motion of the cloud field, independently of the detection and tracking of cloud objects. The semi-Lagrangian framework allows severe storms to be simultaneously detected and tracked in both spatial and temporal dimensions. For the purpose of this framework we have developed a novel Lagrangian convolution method and a number of novel implementations of morphological image operations that account for the motion of observed objects. These novel methods allow the accurate extension of computer vision techniques to the temporal domain for moving objects such as DCCs. By combining this framework with existing methods for detecting DCCs (including detection of growing cores through cloud top cooling and detection of anvil clouds using brightness temperature), we show that the novel framework enables reductions in errors due to both false and missed detections compared to any of the individual methods, reducing the need to compromise when compared with existing frameworks. The novel framework enables the continuous tracking of anvil clouds associated with detected deep convection after convective activity has stopped, enabling the study of the entire life cycle of DCCs and their associated anvils. Furthermore, we expect this framework to be applicable to a wide range of cases including the detection and tracking of low-level clouds and other atmospheric phenomena. In addition, this framework may be used to combine observations from multiple sources, including satellite observations, weather radar and reanalysis model data.

A Lagrangian framework is used to evaluate aerosol–cloud interactions in the U.S. Department of Energy's Energy Exascale Earth System Model (E3SM) version 1 (E3SMv1) for measurements taken at Graciosa Island in the Azores where a U.S. Department of Energy Atmosphere Radiation Measurement (ARM) site is located. This framework uses direct measurements of cloud condensation nuclei (CCN) concentration (instead of relying on satellite retrievals of aerosol optical depth) and incorporates a suite of ground-based ARM measurements, satellite retrievals, and meteorological reanalysis products that when applied to over a 1500 trajectories provides key insights into the evolution of low-level clouds and aerosol radiative forcing that is not feasible from a traditional Eulerian analysis framework. Significantly lower concentrations (40 %) of surface CCN concentration are measured when precipitation rates in 48 h back trajectories average above 1.2 mm d−1 in the Integrated Multi-satellitE Retrievals for Global Precipitation Measurement (IMERG) product. The depletion of CCN concentration when precipitation rates are elevated is nearly twice as large in the ARM observations compared to E3SMv1 simulations. The model CCN concentration bias remains significant despite modifying the autoconversion and accretion rates in warm clouds. As the clouds in trajectories associated with larger surface-based CCN concentration advect away from Graciosa Island, they maintain higher values of droplet number concentrations (Nd) over multiple days in observations and E3SM simulations compared to trajectories that start with lower CCN concentrations. The response remains robust even after controlling for meteorological factors such as lower troposphere stability, the degree of cloud coupling with the surface, and island wake effects. E3SMv1 simulates a multi-day aerosol effect on clouds and a Twomey radiative effect that is within 30 % of the ARM and satellite observations. However, the mean cloud droplet concentration is more than 2–3 times larger than in the observations. While Twomey radiative effects are similar amongst autoconversion and accretion sensitivity experiments, the liquid water path and cloud fraction adjustments are positive when using a regression model as opposed to negative when using the present-day minus pre-industrial aerosol emissions approach. This result suggests that tuning the autoconversion and accretion alone is unlikely to produce the desired aerosol susceptibilities in E3SMv1.

Aerosol–cloud interactions (ACIs) are considered to be the most uncertain driver of present-day radiative forcing due to human activities. The nonlinearity of cloud-state changes to aerosol perturbations make it challenging to attribute causality in observed relationships of aerosol radiative forcing. Using correlations to infer causality can be challenging when meteorological variability also drives both aerosol and cloud changes independently. Natural and anthropogenic aerosol perturbations from well-defined sources provide “opportunistic experiments” (also known as natural experiments) to investigate ACI in cases where causality may be more confidently inferred. These perturbations cover a wide range of locations and spatiotemporal scales, including point sources such as volcanic eruptions or industrial sources, plumes from biomass burning or forest fires, and tracks from individual ships or shipping corridors. We review the different experimental conditions and conduct a synthesis of the available satellite datasets and field campaigns to place these opportunistic experiments on a common footing, facilitating new insights and a clearer understanding of key uncertainties in aerosol radiative forcing. Cloud albedo perturbations are strongly sensitive to background meteorological conditions. Strong liquid water path increases due to aerosol perturbations are largely ruled out by averaging across experiments. Opportunistic experiments have significantly improved process-level understanding of ACI, but it remains unclear how reliably the relationships found can be scaled to the global level, thus demonstrating a need for deeper investigation in order to improve assessments of aerosol radiative forcing and climate change.

We present version 3 (V3) of the Cloud_cci Along-Track Scanning Radiometer (ATSR) and Advanced ATSR (AATSR) data set. The data set was created for the European Space Agency (ESA) Cloud_cci (Climate Change Initiative) programme. The cloud properties were retrieved from the second ATSR (ATSR-2) on board the second European Remote Sensing Satellite (ERS-2) spanning 1995–2003 and the AATSR on board Envisat, which spanned 2002–2012. The data are comprised of a comprehensive set of cloud properties: cloud top height, temperature, pressure, spectral albedo, cloud effective emissivity, effective radius, and optical thickness, alongside derived liquid and ice water path. Each retrieval is provided with its associated uncertainty. The cloud property retrievals are accompanied by high-resolution top- and bottom-of-atmosphere shortwave and longwave fluxes that have been derived from the retrieved cloud properties using a radiative transfer model. The fluxes were generated for all-sky and clear-sky conditions. V3 differs from the previous version 2 (V2) through development of the retrieval algorithm and attention to the consistency between the ATSR-2 and AATSR instruments. The cloud properties show improved accuracy in validation and better consistency between the two instruments, as demonstrated by a comparison of cloud mask and cloud height with co-located CALIPSO data. The cloud masking has improved significantly, particularly in its ability to detect clear pixels. The Kuiper Skill score has increased from 0.49 to 0.66. The cloud top height accuracy is relatively unchanged. The AATSR liquid water path was compared with the Multisensor Advanced Climatology of Liquid Water Path (MAC-LWP) in regions of stratocumulus cloud and shown to have very good agreement and improved consistency between ATSR-2 and AATSR instruments. The correlation with MAC-LWP increased from 0.4 to over 0.8 for these cloud regions. The flux products are compared with NASA Clouds and the Earth's Radiant Energy System (CERES) data, showing good agreement within the uncertainty. The new data set is well suited to a wide range of climate applications, such as comparison with climate models, investigation of trends in cloud properties, understanding aerosol–cloud interactions, and providing contextual information for co-located ATSR-2/AATSR surface temperature and aerosol products. The following new digital identifier has been issued for the Cloud_cci ATSR-2/AATSRv3 data set: https://doi.org/10.5676/DWD/ESA_Cloud_cci/ATSR2-AATSR/V003 (Poulsen et al., 2019).

Abstract Clouds are critical for weather and climate prediction. The multiple scales of cloud processes make simulation difficult. Often models and measurements are used to develop empirical relationships for large‐scale models to be computationally efficient. Machine learning provides another potential tool to improve our empirical parameterizations of clouds. To explore these opportunities, we replace the warm rain formation process in a General Circulation Model (GCM) with a detailed treatment from a bin microphysical model that causes a 400% slowdown in the GCM. We analyze the changes in climate that result from the use of the bin microphysical calculation and find improvements in the rain onset and frequency of light rain compared to high resolution process models and observations. We also find a resulting change in the cloud feedback response of the model to warming, which will significantly impact the climate sensitivity. We then replace the bin microphysical model with several neural networks designed to emulate the autoconversion and accretion rates produced by the bin microphysical model. The neural networks are organized into two stages: the first stage identifies where tendencies will be nonzero (and the sign of the tendency), and the second stage predicts the magnitude of the autoconversion and accretion rates. We describe the risks of overfitting, extrapolation, and linearization by using perfect model experiments with and without the emulator. We can recover the solutions with the emulators in almost all respects, and get simulations that perform as the detailed model, but with the computational cost of the control simulation.

The Community Cloud retrieval for Climate (CC4CL) is a cloud property retrieval system for satellite-based multispectral imagers and is an important component of the Cloud Climate Change Initiative (Cloud_cci) project. In this paper we discuss the optimal estimation retrieval of cloud optical thickness, effective radius and cloud top pressure based on the Optimal Retrieval of Aerosol and Cloud (ORAC) algorithm. Key to this method is the forward model, which includes the clear-sky model, the liquid water and ice cloud models, the surface model including a bidirectional reflectance distribution function (BRDF), and the "fast" radiative transfer solution (which includes a multiple scattering treatment). All of these components and their assumptions and limitations will be discussed in detail. The forward model provides the accuracy appropriate for our retrieval method. The errors are comparable to the instrument noise for cloud optical thicknesses greater than 10. At optical thicknesses less than 10 modeling errors become more significant. The retrieval method is then presented describing optimal estimation in general, the nonlinear inversion method employed, measurement and a priori inputs, the propagation of input uncertainties and the calculation of subsidiary quantities that are derived from the retrieval results. An evaluation of the retrieval was performed using measurements simulated with noise levels appropriate for the MODIS instrument. Results show errors less than 10 % for cloud optical thicknesses greater than 10. Results for clouds of optical thicknesses less than 10 have errors up to 20 %.

Aerosol–cloud interactions (ACIs) are uncertain and the estimates of the ACI effective radiative forcing (ERFaci) magnitude show a large variability. Within the Aerosol_cci project the susceptibility of cloud properties to changes in aerosol properties is derived from the high-resolution AATSR (Advanced Along-Track Scanning Radiometer) data set using the Cloud–Aerosol Pairing Algorithm (CAPA) (as described in our companion paper) and compared to susceptibilities from the global aerosol climate model ECHAM6-HAM2 and MODIS–CERES (Moderate Resolution Imaging Spectroradiometer – Clouds and the Earth's Radiant Energy System) data. For ECHAM6-HAM2 the dry aerosol is analysed to mimic the effect of CAPA. Furthermore the analysis is done for different environmental regimes. The aerosol–liquid water path relationship in ECHAM6-HAM2 is systematically stronger than in AATSR–CAPA data and cannot be explained by an overestimation of autoconversion when using diagnostic precipitation but rather by aerosol swelling in regions where humidity is high and clouds are present. When aerosol water is removed from the analysis in ECHAM6-HAM2 the strength of the susceptibilities of liquid water path, cloud droplet number concentration and cloud albedo as well as ERFaci agree much better with those of AATSR–CAPA or MODIS–CERES. When comparing satellite-derived to model-derived susceptibilities, this study finds it more appropriate to use dry aerosol in the computation of model susceptibilities. We further find that the statistical relationships inferred from different satellite sensors (AATSR–CAPA vs. MODIS–CERES) as well as from ECHAM6-HAM2 are not always of the same sign for the tested environmental conditions. In particular the susceptibility of the liquid water path is negative in non-raining scenes for MODIS–CERES but positive for AATSR–CAPA and ECHAM6-HAM2. Feedback processes like cloud-top entrainment that are missing or not well represented in the model are therefore not well constrained by satellite observations. In addition to aerosol swelling, wet scavenging and aerosol processing have an impact on liquid water path, cloud albedo and cloud droplet number susceptibilities. Aerosol processing leads to negative liquid water path susceptibilities to changes in aerosol index (AI) in ECHAM6-HAM2, likely due to aerosol-size changes by aerosol processing. Our results indicate that for statistical analysis of aerosol–cloud interactions the unwanted effects of aerosol swelling, wet scavenging and aerosol processing need to be minimised when computing susceptibilities of cloud variables to changes in aerosol.

Increased concentrations of aerosol can enhance the albedo of warm low-level cloud. Accurately quantifying this relationship from space is challenging due in part to contamination of aerosol statistics near clouds. Aerosol retrievals near clouds can be influenced by stray cloud particles in areas assumed to be cloud-free, particle swelling by humidification, shadows and enhanced scattering into the aerosol field from (3-D radiative transfer) clouds. To screen for this contamination we have developed a new cloud–aerosol pairing algorithm (CAPA) to link cloud observations to the nearest aerosol retrieval within the satellite image. The distance between each aerosol retrieval and nearest cloud is also computed in CAPA. Results from two independent satellite imagers, the Advanced Along-Track Scanning Radiometer (AATSR) and Moderate Resolution Imaging Spectroradiometer (MODIS), show a marked reduction in the strength of the intrinsic aerosol indirect radiative forcing when selecting aerosol pairs that are located farther away from the clouds (−0.28±0.26 W m−2) compared to those including pairs that are within 15 km of the nearest cloud (−0.49±0.18 W m−2). The larger aerosol optical depths in closer proximity to cloud artificially enhance the relationship between aerosol-loading, cloud albedo, and cloud fraction. These results suggest that previous satellite-based radiative forcing estimates represented in key climate reports may be exaggerated due to the inclusion of retrieval artefacts in the aerosol located near clouds.

The concept of geoengineering by marine cloud brightening is based on seeding marine stratocumulus clouds with sub-micrometer sea-salt particles to enhance the cloud droplet number concentration and cloud albedo, thereby producing a climate cooling effect. The efficacy of this as a strategy for global cooling rests on the extent to which aerosol-perturbed marine clouds will respond with increased albedo. Ship tracks, quasi-linear cloud features prevalent in oceanic regions impacted by ship exhaust, are a well-known manifestation of the effect of aerosol injection on marine clouds. We present here an analysis of the albedo responses in ship tracks, based on in situ aircraft measurements and three years of satellite observations of 589 individual ship tracks. It is found that the sign (increase or decrease) and magnitude of the albedo response in ship tracks depends on the mesoscale cloud structure, the free tropospheric humidity, and cloud top height. In a closed cell structure (cloud cells ringed by a perimeter of clear air), nearly 30% of ship tracks exhibited a decreased albedo. Detailed cloud responses must be accounted for in global studies of the potential efficacy of sea-spray geoengineering as a means to counteract global warming.