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One major source of uncertainty in the cloud-mediated aerosol forcing arises from the magnitude of the cloud liquid water path (LWP) adjustment to aerosol-cloud interactions, which is poorly constrained by observations. Many of the recent satellite-based studies have observed a decreasing LWP as a function of cloud droplet number concentration (CDNC) as the dominating behavior. Estimating the LWP response to the CDNC changes is a complex task since various confounding factors need to be isolated. However, an important aspect has not been sufficiently considered: the propagation of natural spatial variability and errors in satellite retrievals of cloud optical depth and cloud effective radius to estimates of CDNC and LWP. Here we use satellite and simulated measurements to demonstrate that, because of this propagation, even a positive LWP adjustment is likely to be misinterpreted as negative. This biasing effect therefore leads to an underestimate of the aerosol-cloud-climate cooling and must be properly considered in future studies., (© 2022. The Author(s).)

Aerosols have a dimming and cooling effect and change hydrological regimes, thus affecting carbon fluxes, which are sensitive to climate. Aerosols also scatter sunlight, which increases the fraction of diffuse radiation, increasing photosynthesis. There remains no clear conclusion whether the impact of aerosols on land carbon fluxes is larger through diffuse radiation change than through changes in other climate variables. In this study, we quantified the overall physical impacts of anthropogenic aerosols on land C fluxes and explored the contribution from each factor using a set of factorial simulations driven by climate and aerosol data from the IPSL-CM6A-LR experiments during 1850-2014. A newly developed land surface model which distinguishes diffuse and direct radiation in canopy radiation transmission, ORCHIDEE_DF, was used. Specifically, a subgrid scheme was developed to distinguish the cloudy and clear sky conditions. We found that anthropogenic aerosol emissions since 1850 cumulatively enhanced the land C sink by 22.6 PgC. Seventy-eight percent of this C sink enhancement is contributed by aerosol-induced increase in the diffuse radiation fraction, much larger than the effect of the aerosol-induced dimming. The cooling of anthropogenic aerosols has different impacts in different latitudes but overall increases the global land C sink. The dominant role of diffuse radiation changes found in this study implies that future aerosol emissions may have a much stronger impacts on the C cycle through changing radiation quality than through changing climate alone. Earth system models need to consider the diffuse radiation fertilization effect to better evaluate the impacts of climate change mitigation scenarios., (© 2021. The Authors.)

The Coronavirus Disease 2019 (COVID-19) pandemic led to a widespread reduction in aerosol emissions. Using satellite observations and climate model simulations, we study the underlying mechanisms of the large decreases in solar clear-sky reflection (3.8 W m -2 or 7%) and aerosol optical depth (0.16 W m -2 or 32%) observed over the East Asian Marginal Seas in March 2020. By separating the impacts from meteorology and emissions in the model simulations, we find that about one-third of the clear-sky anomalies can be attributed to pandemic-related emission reductions, and the rest to weather variability and long-term emission trends. The model is skillful at reproducing the observed interannual variations in solar all-sky reflection, but no COVID-19 signal is discerned. The current observational and modeling capabilities will be critical for monitoring, understanding, and predicting the radiative forcing and climate impacts of the ongoing crisis., (© 2020. The Authors. This article has been contributed to by US Government employees and their work is in the public domain in the USA.)

Uncertainty in the representation of biomass burning (BB) aerosol composition and optical properties in climate models contributes to a range in modeled aerosol effects on incoming solar radiation. Depending on the model, the top-of-the-atmosphere BB aerosol effect can range from cooling to warming. By relating aerosol absorption relative to extinction and carbonaceous aerosol composition from 12 observational datasets to nine state-of-the-art Earth system models/chemical transport models, we identify varying degrees of overestimation in BB aerosol absorptivity by these models. Modifications to BB aerosol refractive index, size, and mixing state improve the Community Atmosphere Model version 5 (CAM5) agreement with observations, leading to a global change in BB direct radiative effect of -0.07 W m -2 , and regional changes of -2 W m -2 (Africa) and -0.5 W m -2 (South America/Temperate). Our findings suggest that current modeled BB contributes less to warming than previously thought, largely due to treatments of aerosol mixing state.

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., (©2019. The Authors.)

An Amendment to this paper has been published and can be accessed via a link at the top of the paper.

The cooling of the Earth's climate through the effects of anthropogenic aerosols on clouds offsets an unknown fraction of greenhouse gas warming. An increase in the amount of water inside liquid-phase clouds induced by aerosols, through the suppression of rain formation, has been postulated to lead to substantial cooling, which would imply that the Earth's surface temperature is highly sensitive to anthropogenic forcing. Here we provide direct observational evidence that, instead of a strong increase, aerosols cause a relatively weak average decrease in the amount of water in liquid-phase clouds compared with unpolluted clouds. Measurements of polluted clouds downwind of various anthropogenic sources-such as oil refineries, smelters, coal-fired power plants, cities, wildfires and ships-reveal that aerosol-induced cloud-water increases, caused by suppressed rain formation, and decreases, caused by enhanced evaporation of cloud water, partially cancel each other out. We estimate that the observed decrease in cloud water offsets 23% of the global climate-cooling effect caused by aerosol-induced increases in the concentration of cloud droplets. These findings invalidate the hypothesis that increases in cloud water cause a substantial climate cooling effect and translate into reduced uncertainty in projections of future climate.

Aerosol-cloud interaction is the most uncertain mechanism of anthropogenic radiative forcing of Earth's climate, and aerosol-induced cloud water changes are particularly poorly constrained in climate models. By combining satellite retrievals of volcano and ship tracks in stratocumulus clouds, we compile a unique observational dataset and confirm that liquid water path (LWP) responses to aerosols are bidirectional, and on average the increases in LWP are closely compensated by the decreases. Moreover, the meteorological parameters controlling the LWP responses are strikingly similar between the volcano and ship tracks. In stark contrast to observations, there are substantial unidirectional increases in LWP in the Hadley Centre climate model, because the model accounts only for the decreased precipitation efficiency and not for the enhanced entrainment drying. If the LWP increases in the model were compensated by the decreases as the observations suggest, its indirect aerosol radiative forcing in stratocumulus regions would decrease by 45%.

This corrects the article DOI: 10.1038/nature22974.

Aerosols have a potentially large effect on climate, particularly through their interactions with clouds, but the magnitude of this effect is highly uncertain. Large volcanic eruptions produce sulfur dioxide, which in turn produces aerosols; these eruptions thus represent a natural experiment through which to quantify aerosol-cloud interactions. Here we show that the massive 2014-2015 fissure eruption in Holuhraun, Iceland, reduced the size of liquid cloud droplets-consistent with expectations-but had no discernible effect on other cloud properties. The reduction in droplet size led to cloud brightening and global-mean radiative forcing of around -0.2 watts per square metre for September to October 2014. Changes in cloud amount or cloud liquid water path, however, were undetectable, indicating that these indirect effects, and cloud systems in general, are well buffered against aerosol changes. This result will reduce uncertainties in future climate projections, because we are now able to reject results from climate models with an excessive liquid-water-path response.

The ability of 11 models in simulating the aerosol vertical distribution from regional to global scales, as part of the second phase of the AeroCom model intercomparison initiative (AeroCom II), is assessed and compared to results of the first phase. The evaluation is performed using a global monthly gridded data set of aerosol extinction profiles built for this purpose from the CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) Layer Product 3.01. Results over 12 subcontinental regions show that five models improved, whereas three degraded in reproducing the interregional variability in Z α 0-6 km , the mean extinction height diagnostic, as computed from the CALIOP aerosol profiles over the 0-6 km altitude range for each studied region and season. While the models' performance remains highly variable, the simulation of the timing of the Z α 0-6 km peak season has also improved for all but two models from AeroCom Phase I to Phase II. The biases in Z α 0-6 km are smaller in all regions except Central Atlantic, East Asia, and North and South Africa. Most of the models now underestimate Z α 0-6 km over land, notably in the dust and biomass burning regions in Asia and Africa. At global scale, the AeroCom II models better reproduce the Z α 0-6 km latitudinal variability over ocean than over land. Hypotheses for the performance and evolution of the individual models and for the intermodel diversity are discussed. We also provide an analysis of the CALIOP limitations and uncertainties contributing to the differences between the simulations and observations.

Systematic climate shifts have been linked to multidecadal variability in observed sea surface temperatures in the North Atlantic Ocean. These links are extensive, influencing a range of climate processes such as hurricane activity and African Sahel and Amazonian droughts. The variability is distinct from historical global-mean temperature changes and is commonly attributed to natural ocean oscillations. A number of studies have provided evidence that aerosols can influence long-term changes in sea surface temperatures, but climate models have so far failed to reproduce these interactions and the role of aerosols in decadal variability remains unclear. Here we use a state-of-the-art Earth system climate model to show that aerosol emissions and periods of volcanic activity explain 76 per cent of the simulated multidecadal variance in detrended 1860-2005 North Atlantic sea surface temperatures. After 1950, simulated variability is within observational estimates; our estimates for 1910-1940 capture twice the warming of previous generation models but do not explain the entire observed trend. Other processes, such as ocean circulation, may also have contributed to variability in the early twentieth century. Mechanistically, we find that inclusion of aerosol-cloud microphysical effects, which were included in few previous multimodel ensembles, dominates the magnitude (80 per cent) and the spatial pattern of the total surface aerosol forcing in the North Atlantic. Our findings suggest that anthropogenic aerosol emissions influenced a range of societally important historical climate events such as peaks in hurricane activity and Sahel drought. Decadal-scale model predictions of regional Atlantic climate will probably be improved by incorporating aerosol-cloud microphysical interactions and estimates of future concentrations of aerosols, emissions of which are directly addressable by policy actions.

Many atmospheric constituents besides carbon dioxide (CO(2)) contribute to global warming, and it is common to compare their influence on climate in terms of radiative forcing, which measures their impact on the planetary energy budget. A number of recent studies have shown that many radiatively active constituents also have important impacts on the physiological functioning of ecosystems, and thus the 'ecosystem services' that humankind relies upon. CO(2) increases have most probably increased river runoff and had generally positive impacts on plant growth where nutrients are non-limiting, whereas increases in near-surface ozone (O(3)) are very detrimental to plant productivity. Atmospheric aerosols increase the fraction of surface diffuse light, which is beneficial for plant growth. To illustrate these differences, we present the impact on net primary productivity and runoff of higher CO(2), higher near-surface O(3), and lower sulphate aerosols, and for equivalent changes in radiative forcing. We compare this with the impact of climate change alone, arising, for example, from a physiologically inactive gas such as methane (CH(4)). For equivalent levels of change in radiative forcing, we show that the combined climate and physiological impacts of these individual agents vary markedly and in some cases actually differ in sign. This study highlights the need to develop more informative metrics of the impact of changing atmospheric constituents that go beyond simple radiative forcing., (© 2011 The Royal Society)

Plant photosynthesis tends to increase with irradiance. However, recent theoretical and observational studies have demonstrated that photosynthesis is also more efficient under diffuse light conditions. Changes in cloud cover or atmospheric aerosol loadings, arising from either volcanic or anthropogenic emissions, alter both the total photosynthetically active radiation reaching the surface and the fraction of this radiation that is diffuse, with uncertain overall effects on global plant productivity and the land carbon sink. Here we estimate the impact of variations in diffuse fraction on the land carbon sink using a global model modified to account for the effects of variations in both direct and diffuse radiation on canopy photosynthesis. We estimate that variations in diffuse fraction, associated largely with the 'global dimming' period, enhanced the land carbon sink by approximately one-quarter between 1960 and 1999. However, under a climate mitigation scenario for the twenty-first century in which sulphate aerosols decline before atmospheric CO(2) is stabilized, this 'diffuse-radiation' fertilization effect declines rapidly to near zero by the end of the twenty-first century.

Atmospheric aerosols cause scattering and absorption of incoming solar radiation. Additional anthropogenic aerosols released into the atmosphere thus exert a direct radiative forcing on the climate system. The degree of present-day aerosol forcing is estimated from global models that incorporate a representation of the aerosol cycles. Although the models are compared and validated against observations, these estimates remain uncertain. Previous satellite measurements of the direct effect of aerosols contained limited information about aerosol type, and were confined to oceans only. Here we use state-of-the-art satellite-based measurements of aerosols and surface wind speed to estimate the clear-sky direct radiative forcing for 2002, incorporating measurements over land and ocean. We use a Monte Carlo approach to account for uncertainties in aerosol measurements and in the algorithm used. Probability density functions obtained for the direct radiative forcing at the top of the atmosphere give a clear-sky, global, annual average of -1.9 W m(-2) with standard deviation, +/- 0.3 W m(-2). These results suggest that present-day direct radiative forcing is stronger than present model estimates, implying future atmospheric warming greater than is presently predicted, as aerosol emissions continue to decline.