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Eastern China has experienced severe and persistent winter haze episodes in recent years due to intensification of aerosol pollution. In addition to anthropogenic emissions, the winter aerosol pollution over eastern China is associated with unusual meteorological conditions, including weaker wind speeds. Here we show, based on model simulations, that during years with decreased wind speed, large decreases in dust emissions (29%) moderate the wintertime land–sea surface air temperature difference and further decrease winds by −0.06 (±0.05) m s −1 averaged over eastern China. The dust-induced lower winds enhance stagnation of air and account for about 13% of increasing aerosol concentrations over eastern China. Although recent increases in anthropogenic emissions are the main factor causing haze over eastern China, we conclude that natural emissions also exert a significant influence on the increases in wintertime aerosol concentrations, with important implications that need to be taken into account by air quality studies. Anthropogenic aerosol and calm conditions give rise to winter haze episodes in eastern China. Yang et al . show that these weak winds also decrease natural dust emissions, reducing the land–ocean temperature difference and associated winds, enhancing air stagnation and pollution in this region.

Aerosol-cloud interactions remain a major uncertainty in climate research. Studies have indicated that model estimates of cloud susceptibility to aerosols frequently exceed satellite estimates, motivating model reformulations to increase agreement. Here we show that conventional ways of using satellite information to estimate susceptibility can serve as only a weak constraint on models because the estimation is sensitive to errors in the retrieval procedures. Using instrument simulators to investigate differences between model and satellite estimates of susceptibilities, we find that low aerosol loading conditions are not well characterized by satellites, but model clouds are sensitive to aerosol perturbations in these conditions. We quantify the observational requirements needed to constrain models, and find that the nighttime lidar measurements of aerosols provide a better characterization of ten- uous aerosols. We conclude that observational uncertainties and limitations need to be accounted for when assessing the role of aerosols in the climate system.

The effective radiative forcing of anthropogenic aerosols (ERFaer) is an important measure of the anthropogenic aerosol effects simulated by a global climate model. Here we analyze ERFaer simulated by the E3SM version 1 (E3SMv1) atmospheric model using both century-long free-running atmosphere–land simulations and short nudged simulations. We relate the simulated ERFaer to characteristics of the aerosol composition and optical properties, and we evaluate the relationships between key aerosol and cloud properties. In terms of historical changes from the year 1870 to 2014, our results show that the global mean anthropogenic aerosol burden and optical depth increase during the simulation period as expected, but the regional averages show large differences in the temporal evolution. The largest regional differences are found in the emission-induced evolution of the burden and optical depth of the sulfate aerosol: a strong decreasing trend is seen in the Northern Hemisphere high-latitude region after around 1970, while a continued increase is simulated in the tropics. The relationships between key aerosol and cloud properties (relative changes between pre-industrial and present-day conditions) also show evident changes after 1970, diverging from the linear relationships exhibited for the period of 1870–1969. In addition to the regional differences in the simulated relationships, a reduced sensitivity in cloud droplet number and other cloud properties to aerosol perturbations is seen when the aerosol perturbation is large. Consequently, the global annual mean ERFaer magnitude does not increase after around 1970. The ERFaer in E3SMv1 is relatively large compared to the recently published multi-model estimates; the primary reason is the large indirect aerosol effect (i.e., through aerosol–cloud interactions). Compared to other models, E3SMv1 features large relative changes in the cloud droplet effective radius in response to aerosol perturbations. Large sensitivity is also seen in the liquid cloud optical depth, which is determined by changes in both the effective radius and liquid water path. Aerosol-induced changes in liquid and ice cloud properties in E3SMv1 are found to have a strong correlation, as the evolution of anthropogenic sulfate aerosols affects both the liquid cloud formation and the homogeneous ice nucleation in cirrus clouds (that causes a large effect on longwave ERFaer). As suggested by a previous study, the large ERFaer appears to be one of the reasons why the model cannot reproduce the observed global mean temperature evolution in the second half of the 20th century. Sensitivity simulations are performed to understand which parameterization and/or parameter changes have a large impact on the simulated ERFaer. The ERFaer estimates in E3SMv1 for the shortwave and longwave components are sensitive to the parameterization changes in both liquid and ice cloud processes. When the parameterization of ice cloud processes is modified, the top-of-model forcing changes in the shortwave and longwave components largely offset each other, so the net effect is negligible. This suggests that, to reduce the magnitude of the net ERFaer, it would be more effective to reduce the anthropogenic aerosol effect through liquid or mixed-phase clouds.

The new Energy Exascale Earth System Model Version 1 (E3SMv1) developed for the U.S. Department of Energy has significant new treatments of aerosols and light‐absorbing snow impurities as well as their interactions with clouds and radiation. This study describes seven sets of new aerosol‐related treatments (involving emissions, new particle formation, aerosol transport, wet scavenging and resuspension, and snow radiative transfer) and examines how they affect global aerosols and radiative forcing in E3SMv1. Altogether, they give a reduced total aerosol radiative forcing (−1.6 W/m2) and sensitivity in cloud liquid water to aerosols, but an increased sensitivity in cloud droplet size to aerosols. A new approach for H2SO4 production and loss largely reduces a low bias in small particles concentrations and leads to substantial increases in cloud condensation nuclei concentrations and cloud radiative cooling. Emitting secondary organic aerosol precursor gases from elevated sources increases the column burden of secondary organic aerosol, contributing substantially to global clear‐sky aerosol radiative cooling (−0.15 out of −0.5 W/m2). A new treatment of aerosol resuspension from evaporating precipitation, developed to remedy two shortcomings of the original treatment, produces a modest reduction in aerosols and cloud droplets; its impact depends strongly on the model physics and is much stronger in E3SM Version 0. New treatments of the mixing state and optical properties of snow impurities and snow grains introduce a positive present‐day shortwave radiative forcing (0.26 W/m2), but changes in aerosol transport and wet removal processes also affect the concentration and radiative forcing of light‐absorbing impurities in snow/ice. Plain Language Summary Aerosol and aerosol‐cloud interactions continue to be a major uncertainty in Earth system models, impeding their ability to reproduce the observed historical warming and to project changes in global climate and water cycle. The U.S. DOE Energy Exascale Earth System Model version 1 (E3SMv1), a state‐of‐the‐science Earth system model, was developed to use exascale computing to address the grand challenge of actionable predictions of variability and change in the Earth system critical to the energy sector. It has been publicly released with new treatments in many aspects, including substantial modifications to the physical treatments of aerosols in the atmosphere and light‐absorbing impurities in snow/ice, aimed at reducing some known biases or correcting model deficiencies in representing aerosols, their life cycle, and their impacts in various components of the Earth system. Compared to its predecessors (without the new treatments) and observations, E3SMv1 shows improvements in characterizing global distributions of aerosols and their radiative effects. We conduct sensitivity experiments to understand the impact of individual changes and provide guidance for future development of E3SM and other Earth system models. Key Points A description and assessment of new aerosol treatments in the Energy Exascale Earth System Model Version 1 (E3SMv1) is provided Contributions to the total aerosol‐related radiative forcing by individual new treatments and different processes are quantified Some of the new treatments are found to depend on model physics and require further improvement for E3SM or other Earth system models

Aerosol–cloud interactions continue to constitute a major source of uncertainty for the estimate of climate radiative forcing. The variation of aerosol indirect effects (AIE) in climate models is investigated across different dynamical regimes, determined by monthly mean 500 hPa vertical pressure velocity (ω500), lower-tropospheric stability (LTS) and large-scale surface precipitation rate derived from several global climate models (GCMs), with a focus on liquid water path (LWP) response to cloud condensation nuclei (CCN) concentrations. The LWP sensitivity to aerosol perturbation within dynamic regimes is found to exhibit a large spread among these GCMs. It is in regimes of strong large-scale ascent (ω500  <  −25 hPa day−1) and low clouds (stratocumulus and trade wind cumulus) where the models differ most. Shortwave aerosol indirect forcing is also found to differ significantly among different regimes. Shortwave aerosol indirect forcing in ascending regimes is close to that in subsidence regimes, which indicates that regimes with strong large-scale ascent are as important as stratocumulus regimes in studying AIE. It is further shown that shortwave aerosol indirect forcing over regions with high monthly large-scale surface precipitation rate (> 0.1 mm day−1) contributes the most to the total aerosol indirect forcing (from 64 to nearly 100 %). Results show that the uncertainty in AIE is even larger within specific dynamical regimes compared to the uncertainty in its global mean values, pointing to the need to reduce the uncertainty in AIE in different dynamical regimes.

Natural modes of variability on many timescales influence aerosol particle distributions and cloud properties such that isolating statistically significant differences in cloud radiative forcing due to anthropogenic aerosol perturbations (indirect effects) typically requires integrating over long simulations. For state‐of‐the‐art global climate models (GCM), especially those in which embedded cloud‐resolving models replace conventional statistical parameterizations (i.e., multiscale modeling framework, MMF), the required long integrations can be prohibitively expensive. Here an alternative approach is explored, which implements Newtonian relaxation (nudging) to constrain simulations with both pre‐industrial and present‐day aerosol emissions toward identical meteorological conditions, thus reducing differences in natural variability and dampening feedback responses in order to isolate radiative forcing. Ten‐year GCM simulations with nudging provide a more stable estimate of the global‐annual mean net aerosol indirect radiative forcing than do conventional free‐running simulations. The estimates have mean values and 95% confidence intervals of −1.19 ± 0.02 W/m2 and −1.37 ± 0.13 W/m2for nudged and free‐running simulations, respectively. Nudging also substantially increases the fraction of the world's area in which a statistically significant aerosol indirect effect can be detected (66% and 28% of the Earth's surface for nudged and free‐running simulations, respectively). One‐year MMF simulations with and without nudging provide global‐annual mean net aerosol indirect radiative forcing estimates of −0.81 W/m2 and −0.82 W/m2, respectively. These results compare well with previous estimates from three‐year free‐running MMF simulations (−0.83 W/m2), which showed the aerosol‐cloud relationship to be in better agreement with observations and high‐resolution models than in the results obtained with conventional cloud parameterizations. Key Points Nudged simulations provide more stable estimates of aerosol indirect effects Nudging increases the area a statistically significant signal can be detected Nudging enables computation‐expensive GCMs to estimate aerosol indirect effects

This paper presents a satellite-observation-based evaluation of the marine boundary layer (MBL) cloud properties from two Community Atmosphere Model, version 5 (CAM5), simulations, one with the standard parameterization schemes (CAM5–Base) and the other with the Cloud Layers Unified by Binormals scheme (CAM5–CLUBB). When comparing the direct model outputs, the authors find that CAM5–CLUBB produces more MBL clouds, a smoother transition from stratocumulus to cumulus, and a tighter correlation between in-cloud water and cloud fraction than CAM5–Base. In the model-to-observation comparison using the COSP satellite simulators, the authors find that both simulations capture the main features and spatial patterns of the observed cloud fraction from MODIS and shortwave cloud radiative forcing (SWCF) from CERES. However, CAM5–CLUBB suffers more than CAM5–Base from a problem that can be best summarized as “undetectable” clouds (i.e., a significant fraction of simulated MBL clouds are thinner than the MODIS detection threshold). This issue leads to a smaller COSP–MODIS cloud fraction and a weaker SWCF in CAM5–CLUBB than the observations and also CAM5–Base in the tropical descending regions. Finally, the authors compare modeled radar reflectivity with CloudSat observations and find that both simulations, especially CAM5–CLUBB, suffer from an excessive drizzle problem. Further analysis reveals that the subgrid precipitation enhancement factors in CAM5–CLUBB are unrealistically large, which makes MBL clouds precipitate too excessively, and in turn results in too many undetectable thin clouds.

A prognostic equation for ice crystal number concentration together with an ice nucleation scheme are implemented in the National Center for Atmospheric Research (NCAR) Community Atmospheric Model version 3 (CAM3) with the aim of studying the indirect effect of aerosols on cold clouds. The effective radius of ice crystals, which is used in the radiation and gravitational settlement calculations, is now calculated from model-predicted mass and number of ice crystals rather than diagnosed as a function of temperature. A water vapor deposition scheme is added to replace the condensation and evaporation (C–E) in the standard CAM3 for ice clouds. The repartitioning of total water into liquid and ice in mixed-phase clouds as a function of temperature is removed, and ice supersaturation is allowed. The predicted ice water content in the modified CAM3 is in better agreement with theAuraMicrowave Limb Sounder (MLS) data than that in the standard CAM3. The cirrus cloud fraction near the tropical tropopause, which is underestimated in the standard CAM3 as revealed through comparison with the Stratospheric Aerosol and Gas Experiment II (SAGE II) data, is increased by 20%–30%, and the cold temperature bias there is reduced by 1–2 K. However, an increase in the cloud fraction in polar regions makes the underestimation (by ~20 W m−2) of downwelling shortwave radiation in the standard CAM3 even worse. A sensitivity test reducing the threshold relative humidity with respect to ice (RH i ) for heterogeneous ice nucleation from 120% to 105% (representing nearly perfect ice nuclei) increases the global cloud cover by 1.4%, temperature near the tropical tropopause by 4–5 K, and water vapor in the stratosphere by 50%–80%.

Remote sensing observations of aerosol from surface and satellite instruments are extensively used for atmospheric and climate research. From passive sensors, the apparent cloud‐free atmosphere in the vicinity of clouds often appears to be brighter than further away from the clouds, leading to an increase in the retrieved aerosol optical depth (τ). Mechanisms contributing to this enhancement or increase, including contamination by undetected clouds, hygroscopic growth of aerosol particles, and meteorological conditions, have been debated in recent literature, but the extent to which each of these factors influence the observed enhancement (Δτ) is poorly known. Here we used 11 years of daily global observations at 10 × 10 km2 resolution from the MODIS on the NASA Terra satellite to quantify τ as a function of cloud fraction (CF). Our analysis reveals that, averaged over the globe, the clear sky τ is enhanced by Δτ = 0.05 in cloudy conditions (CF = 0.8–0.9). This enhancement in Δτ corresponds to relative enhancement of 25% in cloudy conditions (CF = 0.8–0.9) compared with relatively clear conditions (CF = 0.1–0.2). Unlike the absolute enhancement Δτ, the relative increase in τis rather consistent in all seasons and is 25–35% in the subtropics and 15–25% at mid and higher latitudes. Using a simple Gaussian probability density function model to connect cloud cover and the distribution of relative humidity, we argue that much of the enhancement is consistent with aerosol hygroscopic growth in the humid environment surrounding clouds. Consideration of these cloud‐dependentτeffects will facilitate understanding aerosol‐cloud interactions and reduce the uncertainty in estimates of aerosol radiative forcing by global climate models. Key Points Global AOD increase is 25% in presence of clouds Relative enhancement in AOD is 25‐35% in the subtropics Relative enhancement in AOD is 15‐25% in mid and higher latitudes

Radiative forcing induced by soot on snow is an important anthropogenic forcing affecting the global climate. In this study we simulated the deposition of soot aerosol on snow and the resulting impact on snowpack and the hydrological cycle in the western United States. A year‐long simulation was performed using the chemistry version of the Weather Research and Forecasting model (WRF‐Chem) to determine the soot deposition, followed by three simulations using WRF in meteorology‐only mode, with and without the soot‐induced snow albedo perturbations. The chemistry simulation shows large spatial variability in soot deposition that reflects the localized emissions and the influence of the complex terrain. The soot‐induced snow albedo perturbations increase the surface net solar radiation flux during late winter to early spring, increase the surface air temperature, and reduce the snow accumulation and spring snowmelt. These effects are stronger over the central Rockies and southern Alberta, where soot deposition and snowpack overlap the most. The indirect forcing of soot accelerates snowmelt and alters stream flows, including a trend toward earlier melt dates in the western United States. The soot‐induced albedo reduction initiates a positive feedback process whereby dirty snow absorbs more solar radiation, heating the surface and warming the air. This warming causes reduced snow depth and fraction, which further reduces the regional surface albedo for the snow‐covered regions. For a doubled snow albedo perturbation, the change to surface energy and temperature is around 50–80%; however, snowpack reduction is nonlinearly accelerated.