Aerosols interact with radiation and clouds. Substantial progress made over the past 40 years in observing, understanding, and modeling these processes helped quantify the imbalance in the Earth's radiation budget caused by anthropogenic aerosols, called aerosol radiative forcing, but uncertainties remain large. This review provides a new range of aerosol radiative forcing over the industrial era based on multiple, traceable, and arguable lines of evidence, including modeling approaches, theoretical considerations, and observations. Improved understanding of aerosol absorption and the causes of trends in surface radiative fluxes constrain the forcing from aerosol‐radiation interactions. A robust theoretical foundation and convincing evidence constrain the forcing caused by aerosol‐driven increases in liquid cloud droplet number concentration. However, the influence of anthropogenic aerosols on cloud liquid water content and cloud fraction is less clear, and the influence on mixed‐phase and ice clouds remains poorly constrained. Observed changes in surface temperature and radiative fluxes provide additional constraints. These multiple lines of evidence lead to a 68% confidence interval for the total aerosol effective radiative forcing of ‐1.6 to ‐0.6 W m⁻², or ‐2.0 to ‐0.4 W m⁻² with a 90% likelihood. Those intervals are of similar width to the last Intergovernmental Panel on Climate Change assessment but shifted toward more negative values. The uncertainty will narrow in the future by continuing to critically combine multiple lines of evidence, especially those addressing industrial‐era changes in aerosol sources and aerosol effects on liquid cloud amount and on ice clouds.

Atmospheric aerosols, suspended solid and liquid particles, act as nucleation sites for cloud drop formation, affecting clouds and cloud properties—ultimately influencing the cloud dynamics, lifetime, water path, and areal extent that determine the reflectivity (albedo) of clouds. The concentration N_d of droplets in clouds that influences planetary albedo is sensitive to the availability of aerosol particles on which the droplets form. Natural aerosol concentrations affect not only cloud properties themselves but also modulate the sensitivity of clouds to changes in anthropogenic aerosols. It is shown that modeled natural aerosols, principally marine biogenic primary and secondary aerosol sources, explain more than half of the spatiotemporal variability in satellite-observed N_d. Enhanced N_d is spatially correlated with regions of high chlorophyll a, and the spatiotemporal variability in N_d is found to be driven primarily by high concentrations of sulfate aerosol at lower Southern Ocean latitudes (35^o to 45^oS) and by organic matter in sea spray aerosol at higher latitudes (45^o to 55^oS). Biogenic sources are estimated to increase the summertime mean reflected solar radiation in excess of 10 W m^–2 over parts of the Southern Ocean, which is comparable to the annual mean increases expected from anthropogenic aerosols over heavily polluted regions of the Northern Hemisphere.

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.

In this study, it is shown that CMIP5 global climate models (GCMs) that convert supercooled water to ice at relatively warm temperatures tend to have a greater mean‐state cloud fraction and more negative cloud feedback in the middle and high latitude Southern Hemisphere. We investigate possible reasons for these relationships by analyzing the mixed‐phase parameterizations in 26 GCMs. The atmospheric temperature where ice and liquid are equally prevalent (T5050) is used to characterize the mixed‐phase parameterization in each GCM. Liquid clouds have a higher albedo than ice clouds, so, all else being equal, models with more supercooled liquid water would also have a higher planetary albedo. The lower cloud fraction in these models compensates the higher cloud reflectivity and results in clouds that reflect shortwave radiation (SW) in reasonable agreement with observations, but gives clouds that are too bright and too few. The temperature at which supercooled liquid can remain unfrozen is strongly anti‐correlated with cloud fraction in the climate mean state across the model ensemble, but we know of no robust physical mechanism to explain this behavior, especially because this anti‐correlation extends through the subtropics. A set of perturbed physics simulations with the Community Atmospheric Model Version 4 (CAM4) shows that, if its temperature‐dependent phase partitioning is varied and the critical relative humidity for cloud formation in each model run is also tuned to bring reflected SW into agreement with observations, then cloud fraction increases and liquid water path (LWP) decreases with T5050, as in the CMIP5 ensemble.

Increasing optical depth poleward of 45° is a robust response to warming in global climate models. Much of this cloud optical depth increase has been hypothesized to be due to transitions from ice‐dominated to liquid‐dominated mixed‐phase cloud. In this study, the importance of liquid‐ice partitioning for the optical depth feedback is quantified for 19 Coupled Model Intercomparison Project Phase 5 models. All models show a monotonic partitioning of ice and liquid as a function of temperature, but the temperature at which ice and liquid are equally mixed (the glaciation temperature) varies by as much as 40 K across models. Models that have a higher glaciation temperature are found to have a smaller climatological liquid water path (LWP) and condensed water path and experience a larger increase in LWP as the climate warms. The ice‐liquid partitioning curve of each model may be used to calculate the response of LWP to warming. It is found that the repartitioning between ice and liquid in a warming climate contributes at least 20% to 80% of the increase in LWP as the climate warms, depending on model. Intermodel differences in the climatological partitioning between ice and liquid are estimated to contribute at least 20% to the intermodel spread in the high‐latitude LWP response in the mixed‐phase region poleward of 45°S. It is hypothesized that a more thorough evaluation and constraint of global climate model mixed‐phase cloud parameterizations and validation of the total condensate and ice‐liquid apportionment against observations will yield a substantial reduction in model uncertainty in the high‐latitude cloud response to warming.

The change in planetary albedo due to aerosol−cloud interactions during the industrial era is the leading source of uncertainty in inferring Earth’s climate sensitivity to increased greenhouse gases from the historical record. The variable that controls aerosol−cloud interactions in warm clouds is droplet number concentration. Global climate models demonstrate that the present-day hemispheric contrast in cloud droplet number concentration between the pristine Southern Hemisphere and the polluted Northern Hemisphere oceans can be used as a proxy for anthropogenically driven change in cloud droplet number concentration. Remotely sensed estimates constrain this change in droplet number concentration to be between 8 cm⁻³ and 24 cm⁻³. By extension, the radiative forcing since 1850 from aerosol−cloud interactions is constrained to be −1.2 W⋅m⁻² to −0.6 W⋅m⁻². The robustness of this constraint depends upon the assumption that pristine Southern Ocean droplet number concentration is a suitable proxy for preindustrial concentrations. Droplet number concentrations calculated from satellite data over the Southern Ocean are high in austral summer. Near Antarctica, they reach values typical of Northern Hemisphere polluted outflows. These concentrations are found to agree with several in situ datasets. In contrast, climate models show systematic underpredictions of cloud droplet number concentration across the Southern Ocean. Near Antarctica, where precipitation sinks of aerosol are small, the underestimation by climate models is particularly large. This motivates the need for detailed process studies of aerosol production and aerosol−cloud interactions in pristine environments. The hemispheric difference in satellite estimated cloud droplet number concentration implies preindustrial aerosol concentrations were higher than estimated by most models. Significance Enhancement of aerosol that can nucleate cloud droplets increases the droplet number concentration and albedo of clouds. This increases the amount of sunlight reflected to space. Uncertainty in how aerosol−cloud interactions over the industrial period have increased planetary albedo by this mechanism leads to significant uncertainty in climate projections. Our work presents a method for observationally constraining the change in albedo due to anthropogenic aerosol emissions: a hemispheric difference in remotely sensed cloud droplet number between the pristine Southern Ocean (a preindustrial proxy) and the polluted Northern Hemisphere. Application of this constraint to climate models reduces the range of estimated albedo change since industrialization and suggests current models underpredict cloud droplet number concentration in the preindustrial era.