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.

The impact of aerosols on cloud properties is one of the largest uncertainties in the anthropogenic radiative forcing of the climate. Significant progress has been made in constraining this forcing using observations, but uncertainty remains, particularly in the magnitude of cloud rapid adjustments to aerosol perturbations. Cloud liquid water path (LWP) is the leading control on liquid-cloud albedo, making it important to observationally constrain the aerosol impact on LWP. Previous modelling and observational studies have shown that multiple processes play a role in determining the LWP response to aerosol perturbations, but that the aerosol effect can be difficult to isolate. Following previous studies using mediating variables, this work investigates use of the relationship between cloud droplet number concentration (N_d) and LWP for constraining the role of aerosols. Using joint-probability histograms to account for the non-linear relationship, this work finds a relationship that is broadly consistent with previous studies. There is significant geographical variation in the relationship, partly due to role of meteorological factors (particularly relative humidity). The N_d–LWP relationship is negative in the majority of regions, suggesting that aerosol-induced LWP reductions could offset a significant fraction of the instantaneous radiative forcing from aerosol–cloud interactions (RFaci). However, variations in the N_d–LWP relationship in response to volcanic and shipping aerosol perturbations indicate that the N_d–LWP relationship overestimates the causal N_d impact on LWP due to the role of confounding factors. The weaker LWP reduction implied by these “natural experiments” means that this work provides an upper bound to the radiative forcing from aerosol-induced changes in the LWP.

Aerosol‐cloud interactions have the potential to modify many different cloud properties. There is significant uncertainty in the strength of these aerosol‐cloud interactions in analyses of observational data, partly due to the difficulty in separating aerosol effects on clouds from correlations generated by local meteorology. The relationship between aerosol and cloud fraction (CF) is particularly important to determine, due to the strong correlation of CF to other cloud properties and its large impact on radiation. It has also been one of the hardest to quantify from satellites due to the strong meteorological covariations involved. This work presents a new method to analyze the relationship between aerosol optical depth (AOD) and CF. By including information about the cloud droplet number concentration (CDNC), the impact of the meteorological covariations is significantly reduced. This method shows that much of the AOD‐CF correlation is explained by relationships other than that mediated by CDNC. By accounting for these, the strength of the global mean AOD‐CF relationship is reduced by around 80%. This suggests that the majority of the AOD‐CF relationship is due to meteorological covariations, especially in the shallow cumulus regime. Requiring CDNC to mediate the AOD‐CF relationship implies an effective anthropogenic radiative forcing from an aerosol influence on liquid CF of −0.48 W m⁻² (−0.1 to −0.64 W m⁻²), although some uncertainty remains due to possible biases in the CDNC retrievals in broken cloud scenes.

Around 5 % of anthropogenic radiative forcing (RF) is attributed to aviation CO₂ and non-CO₂ impacts. This paper quantifies aviation emissions and contrail climate forcing in the North Atlantic, one of the world's busiest air traffic corridors, over 5 years. Between 2016 and 2019, growth in CO₂ (+3.13 % yr⁻¹) and nitrogen oxide emissions (+4.5 % yr⁻¹) outpaced increases in flight distance (+3.05 % yr⁻¹). Over the same period, the annual mean contrail cirrus net RF (204–280 mW m⁻²) showed significant inter-annual variability caused by variations in meteorology. Responses to COVID-19 caused significant reductions in flight distance travelled (−66 %), CO₂ emissions (−71 %) and the contrail net RF (−66 %) compared with the prior 1-year period. Around 12 % of all flights in this region cause 80 % of the annual contrail energy forcing, and the factors associated with strongly warming/cooling contrails include seasonal changes in meteorology and radiation, time of day, background cloud fields, and engine-specific non-volatile particulate matter (nvPM) emissions. Strongly warming contrails in this region are generally formed in wintertime, close to the tropopause, between 15:00 and 04:00 UTC, and above low-level clouds. The most strongly cooling contrails occur in the spring, in the upper troposphere, between 06:00 and 15:00 UTC, and without lower-level clouds. Uncertainty in the contrail cirrus net RF (216–238 mW m⁻²) arising from meteorology in 2019 is smaller than the inter-annual variability. The contrail RF estimates are most sensitive to the humidity fields, followed by nvPM emissions and aircraft mass assumptions. This longitudinal evaluation of aviation contrail impacts contributes a quantified understanding of inter-annual variability and informs strategies for contrail mitigation.

The Twomey effect describes the radiative forcing associated with a change in cloud albedo due to an increase in anthropogenic aerosol emissions. It is driven by the perturbation in cloud droplet number concentration (ΔN_d, ant) in liquid-water clouds and is currently understood to exert a cooling effect on climate. The Twomey effect is the key driver in the effective radiative forcing due to aerosol–cloud interactions, but rapid adjustments also contribute. These adjustments are essentially the responses of cloud fraction and liquid water path to ΔN_d, ant and thus scale approximately with it. While the fundamental physics of the influence of added aerosol particles on the droplet concentration (N_d) is well described by established theory at the particle scale (micrometres), how this relationship is expressed at the large-scale (hundreds of kilometres) perturbation, ΔN_d, ant, remains uncertain. The discrepancy between process understanding at particle scale and insufficient quantification at the climate-relevant large scale is caused by co-variability of aerosol particles and updraught velocity and by droplet sink processes. These operate at scales on the order of tens of metres at which only localised observations are available and at which no approach yet exists to quantify the anthropogenic perturbation. Different atmospheric models suggest diverse magnitudes of the Twomey effect even when applying the same anthropogenic aerosol emission perturbation. Thus, observational data are needed to quantify and constrain the Twomey effect. At the global scale, this means satellite data. There are four key uncertainties in determining ΔN_d, ant, namely the quantification of (i) the cloud-active aerosol – the cloud condensation nuclei (CCN) concentrations at or above cloud base, (ii) N_d, (iii) the statistical approach for inferring the sensitivity of N_d to aerosol particles from the satellite data and (iv) uncertainty in the anthropogenic perturbation to CCN concentrations, which is not easily accessible from observational data. This review discusses deficiencies of current approaches for the different aspects of the problem and proposes several ways forward: in terms of CCN, retrievals of optical quantities such as aerosol optical depth suffer from a lack of vertical resolution, size and hygroscopicity information, non-direct relation to the concentration of aerosols, difficulty to quantify it within or below clouds, and the problem of insufficient sensitivity at low concentrations, in addition to retrieval errors. A future path forward can include utilising co-located polarimeter and lidar instruments, ideally including high-spectral-resolution lidar capability at two wavelengths to maximise vertically resolved size distribution information content. In terms of N_d, a key problem is the lack of operational retrievals of this quantity and the inaccuracy of the retrieval especially in broken-cloud regimes. As for the N_d-to-CCN sensitivity, key issues are the updraught distributions and the role of N_d sink processes, for which empirical assessments for specific cloud regimes are currently the best solutions. These considerations point to the conclusion that past studies using existing approaches have likely underestimated the true sensitivity and, thus, the radiative forcing due to the Twomey effect.

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.