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 cloud droplet number concentration (N_d) is of central interest to improve the understanding of cloud physics and for quantifying the effective radiative forcing by aerosol‐cloud interactions. Current standard satellite retrievals do not operationally provide N_d, but it can be inferred from retrievals of cloud optical depth (τ_c) cloud droplet effective radius (r_e) and cloud top temperature. This review summarizes issues with this approach and quantifies uncertainties. A total relative uncertainty of 78% is inferred for pixel‐level retrievals for relatively homogeneous, optically thick and unobscured stratiform clouds with favorable viewing geometry. The uncertainty is even greater if these conditions are not met. For averages over 1° ×1° regions the uncertainty is reduced to 54% assuming random errors for instrument uncertainties. In contrast, the few evaluation studies against reference in situ observations suggest much better accuracy with little variability in the bias. More such studies are required for a better error characterization. N_d uncertainty is dominated by errors in r_e, and therefore, improvements in r_e retrievals would greatly improve the quality of the N_d retrievals. Recommendations are made for how this might be achieved. Some existing N_d data sets are compared and discussed, and best practices for the use of N_d data from current passive instruments (e.g., filtering criteria) are recommended. Emerging alternative N_d estimates are also considered. First, new ideas to use additional information from existing and upcoming spaceborne instruments are discussed, and second, approaches using high‐quality ground‐based observations are examined.

A climatology of thermodynamic phase of precipitating cloud is presented derived from global—land and ocean—, retrievals from Cloudsat, CALIPSO, and Moderate Resolution Imaging Spectroradiometer. Like precipitation rate, precipitation frequency is dominated by warm rain, defined as rain produced via the liquid phase only, over the tropical oceans outside the Intertropical Convergence Zone and by cold rain, produced via the ice phase, over the midlatitude oceans and continents. Warm rain is very infrequent over the continents, with significant warm rain found only in onshore flow in the tropics, and over India, China, and Indochina. Comparison of the properties of precipitating and nonprecipitating warm clouds shows that the scarcity of warm rain over land can be explained by smaller effective radii in continental clouds that delay the onset of precipitation. The results highlight the importance of ice‐phase processes for the global hydrological cycle and may lead to an improved parameterization of precipitation in general circulation models.

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.

Large‐eddy simulations (LES) with the new ICOsahedral Non‐hydrostatic atmosphere model (ICON) covering Germany are evaluated for four days in spring 2013 using observational data from various sources. Reference simulations with the established Consortium for Small‐scale Modelling (COSMO) numerical weather prediction model and further standard LES codes are performed and used as a reference. This comprehensive evaluation approach covers multiple parameters and scales, focusing on boundary‐layer variables, clouds and precipitation. The evaluation points to the need to work on parametrizations influencing the surface energy balance, and possibly on ice cloud microphysics. The central purpose for the development and application of ICON in the LES configuration is the use of simulation results to improve the understanding of moist processes, as well as their parametrization in climate models. The evaluation thus aims at building confidence in the model's ability to simulate small‐ to mesoscale variability in turbulence, clouds and precipitation. The results are encouraging: the high‐resolution model matches the observed variability much better at small‐ to mesoscales than the coarser resolved reference model. In its highest grid resolution, the simulated turbulence profiles are realistic and column water vapour matches the observed temporal variability at short time‐scales. Despite being somewhat too large and too frequent, small cumulus clouds are well represented in comparison with satellite data, as is the shape of the cloud size spectrum. Variability of cloud water matches the satellite observations much better in ICON than in the reference model. In this sense, it is concluded that the model is fit for the purpose of using its output for parametrization development, despite the potential to improve further some important aspects of processes that are also parametrized in the high‐resolution model.

This study presents airborne in situ and satellite remote sensing climatologies of cirrus clouds and humidity. The climatologies serve as a guide to the properties of cirrus clouds, with the new in situ database providing detailed insights into boreal midlatitudes and the tropics, while the satellite-borne data set offers a global overview. To this end, an extensive, quality-checked data archive, the Cirrus Guide II in situ database, is created from airborne in situ measurements during 150 flights in 24 campaigns. The archive contains meteorological parameters, ice water content (IWC), ice crystal number concentration (N_ice), ice crystal mean mass radius (R_ice), relative humidity with respect to ice (RH_ice), and water vapor mixing ratio (H₂O) for each of the flights. Depending on the parameter, the database has been extended by about a factor of 5–10 compared to earlier studies. As one result of our investigation, we show that the medians of N_ice, R_ice, and RH_ice have distinct patterns in the IWC–T parameter space. Lookup tables of these variables as functions of IWC and T can be used to improve global model cirrus representation and remote sensing retrieval methods. Another outcome of our investigation is that across all latitudes, the thicker liquid-origin cirrus predominate at lower altitudes, while at higher altitudes the thinner in situ-origin cirrus prevail. Further, examination of the radiative characteristics of in situ-origin and liquid-origin cirrus shows that the in situ-origin cirrus only slightly warm the atmosphere, while liquid-origin cirrus have a strong cooling effect. An important step in completing the Cirrus Guide II is the provision of the global cirrus N_ice climatology, derived by means of the retrieval algorithm DARDAR-Nice from 10 years of cirrus remote sensing observations from satellite. The in situ measurement database has been used to evaluate and improve the satellite observations. We found that the global median N_ice from satellite observations is almost 2 times higher than the in situ median and increases slightly with decreasing temperature. N_ice medians of the most frequently occurring cirrus sorted by geographical regions are highest in the tropics, followed by austral and boreal midlatitudes, Antarctica, and the Arctic. Since the satellite climatologies enclose the entire spatial and temporal N_ice occurrence, we could deduce that half of the cirrus are located in the lowest, warmest (224–242 K) cirrus layer and contain a significant amount of liquid-origin cirrus. A specific highlight of the study is the in situ observations of cirrus and humidity in the Asian monsoon anticyclone and the comparison to the surrounding tropics. In the convectively very active Asian monsoon, peak values of N_ice and IWC of 30 cm⁻³ and 1000 ppmv are detected around the cold point tropopause (CPT). Above the CPT, ice particles that are convectively injected can locally add a significant amount of water available for exchange with the stratosphere. We found IWCs of up to 8 ppmv in the Asian monsoon in comparison to only 2 ppmv in the surrounding tropics. Also, the highest RH_ice values (120 %–150 %) inside of clouds and in clear sky are observed around and above the CPT. We attribute this to the high H₂O mixing ratios (typically 3–5 ppmv) observed in the Asian monsoon compared to 1.5 to 3 ppmv found in the tropics. Above the CPT, supersaturations of 10 %–20 % are observed in regions of weak convective activity and up to about 50 % in the Asian monsoon. This implies that the water available for transport into the stratosphere might be higher than the expected saturation value.