Summary (149 words of referenced text): 46The climate impact of aerosols is highly uncertain owing primarily to their poorly quantified 47 influence on cloud properties. During 2014-15, a fissure eruption in Holuhraun (Iceland) 48 emitted huge quantities of sulphur dioxide, resulting in significant reductions in liquid cloud 49 droplet size. Using satellite observations and detailed modelling, we estimate a global mean 50 radiative forcing from the resulting aerosol-induced cloud brightening for the time of the 51 eruption of around -0.2 W.m -2 . Changes in cloud amount or liquid water path are 52 undetectable, indicating that these aerosol-cloud indirect effects are modest. It supports the 53 idea that cloud systems are well buffered against aerosol changes as only impacts on cloud 54 effective radius appear relevant from a climate perspective, thus providing a strong constraint 55 on aerosol-cloud interactions. This result will reduce uncertainties in future climate 56 projections as we are able to reject the results from climate models with an excessive liquid 57 water path response. 58 59Main Text: (3103 words of referenced text, including concluding paragraph) 60 The 2014-15 eruption at Holuhraun (486 words of referenced text): 61Anthropogenic emissions that affect climate are not just confined to greenhouse gases. 62Sulphur dioxide and other pollutants form atmospheric aerosols that can scatter and absorb 63 sunlight and can influence the properties of clouds, modulating the Earth-atmosphere energy 64 balance. Aerosols act as cloud condensation nuclei (CCN); an increase in CCN translates into 65 a higher number of smaller, more reflective cloud droplets that scatter more sunlight back to 66 space 1 (the ÔfirstÕ indirect effect of aerosols). Smaller cloud droplets decrease the efficiency 67 of collision-coalescence processes that are pivotal in rain initiation, thus aerosol-influenced 68 clouds may retain more liquid water and extend coverage/lifetime 2,3 (the ÔsecondÕ or Ôcloud 69 lifetimeÕ indirect effect). Aerosols usually co-vary with key environmental variables making 70 it difficult to disentangle aerosol-cloud impacts from meteorological variability [4][5][6] . 71Additionally, clouds themselves are complex transient systems subject to dynamical 72 feedbacks (e.g. cloud top entrainment/evaporation, invigoration of convection) which 73 influence cloud response [7][8][9][10][11][12] . These aspects present great challenges in evaluating and 74 constraining aerosol-cloud interactions (ACI) in General Circulation Models (GCM) 13-17 , 75 with particular contentious debate surrounding the relative importance of these feedback 76 mechanisms. 77Nonetheless, anthropogenic aerosol emissions are thought to cool the Earth via indirect 78 effects 17 , but the uncertainty ranges from -1.2 to -0.0 W.m -2 (90% confidence interval) due to 79 i) a lack of characterization of the pre-industrial aerosol state 15,18,19 , and ii) model parametric 80 and structural errors in representing cloud responses to aerosol chan...

Sulfate and organic mass in sea spray explain more than half of the variability in Southern Ocean cloud droplet concentration.

Abstract. In this paper we use a novel observational approach to investigate MODIS satellite retrieval biases of τ and r e (using three different MODIS bands: 1.6, 2.1 and 3.7 µm, denoted as r e1.6 , r e2.1 and r e3.7 , respectively) that occur at high solar zenith angles (θ 0 ) and how they affect retrievals of cloud droplet concentration (N d ). Utilizing the large number of overpasses for polar regions and the diurnal variation of θ 0 we estimate biases in the above quantities for an open ocean region that is dominated by low level stratiform clouds.We find that the mean τ is fairly constant between θ 0 = 50 • and ∼65-70 • , but then increases rapidly with an increase of over 70 % between the lowest and highest θ 0 . The r e2.1 and r e3.7 decrease with θ 0 , with effects also starting at around θ 0 =65-70 • . At low θ 0 , the r e values from the three different MODIS bands agree to within around 0.2 µm, whereas at high θ 0 the spread is closer to 1 µm. The percentage changes of r e with θ 0 are considerably lower than those for τ , being around 5 % and 7 % for r e2.1 and r e3.7 . For r e1.6 there was very little change with θ 0 . Evidence is provided that these changes are unlikely to be due to any physical diurnal cycle.The increase in τ and decrease in r e both contribute to an overall increase in N d of 40-70 % between low and high θ 0 . Whilst the overall r e changes are quite small, they are not insignificant for the calculation of N d ; we find that the contributions to N d biases from the τ and r e biases were roughly comparable for r e3.7 , although for the other r e bands the τ changes were considerably more important. Also, when considering only the clouds with the more heterogeneous tops, the importance of the r e biases was considerably enhanced for both r e2.1 and r e3.7 .When using the variability of 1 km resolution τ data (γ τ ) as a heterogeneity parameter we obtained the expected result of increasing differences in τ between high and low θ 0 as heterogeneity increased, which was not the case when using the variability of 5 km resolution cloud top temperature (σ CTT ), suggesting that γ τ is a better predictor of τ biases at high θ 0 than σ CTT . For a given θ 0 , large decreases in r e were observed as the cloud top heterogeneity changed from low to high values, although it is possible that physical changes to the clouds associated with cloud heterogeneity variation may account for some of this. However, for a given cloud top heterogeneity we find that the value of θ 0 affects the sign and magnitude of the relative differences between r e1.6 , r e2.1 and r e3.7 , which has implications for attempts to retrieve vertical cloud information using the different MODIS bands. The relatively larger decrease in r e3.7 and the lack of change of r e1.6 with both θ 0 and cloud top heterogeneity suggest that r e3.7 is more prone to retrieval biases due to high θ 0 than the other bands. We discuss some possible reasons for this.Our results have important implications for individual MODIS swaths at high θ 0...

Aerosol processes and, in particular, aerosol‐cloud interactions cut across the traditional physical‐Earth system boundary of coupled Earth system models and remain one of the key uncertainties in estimating anthropogenic radiative forcing of climate. Here we calculate the historical aerosol effective radiative forcing (ERF) in the HadGEM3‐GA7 climate model in order to assess the suitability of this model for inclusion in the UK Earth system model, UKESM1. The aerosol ERF, calculated for the year 2000 relative to 1850, is large and negative in the standard GA7 model leading to an unrealistic negative total anthropogenic forcing over the twentieth century. We show how underlying assumptions and missing processes in both the physical model and aerosol parameterizations lead to this large aerosol ERF. A number of model improvements are investigated to assess their impact on the aerosol ERF. These include an improved representation of cloud droplet spectral dispersion, updates to the aerosol activation scheme, and black carbon optical properties. One of the largest contributors to the aerosol forcing uncertainty is insufficient knowledge of the preindustrial aerosol climate. We evaluate the contribution of uncertainties in the natural marine emissions of dimethyl sulfide and organic aerosol to the ERF. The combination of model improvements derived from these studies weakens the aerosol ERF by up to 50% of the original value and leads to a total anthropogenic historical forcing more in line with assessed values.

SignificanceSimulated clouds over the Southern Ocean reflect too little solar radiation compared with observations, which results in errors in simulated surface temperatures and in many other important features of the climate system. Our results show that the radiative properties of the most biased types of clouds in cyclonic systems are highly sensitive to the concentration of ice-nucleating particles. The uniquely low concentrations of ice-nucleating particles in this remote marine environment strongly inhibit precipitation and allow much brighter clouds to be sustained.

Aerosol‐cloud interactions (ACI) represent a significant source of forcing uncertainty in global climate models (GCMs). Estimates of radiative forcing due to ACI in Fifth Assessment Report range from −0.5 to −2.5 W m−2. A portion of this uncertainty is related to the first indirect, or Twomey, effect whereby aerosols act as nuclei for cloud droplets to condense upon. At constant liquid water content this increases the number of cloud droplets (Nd) and thus increases the cloud albedo. In this study we use remote‐sensing estimates of Nd within stratocumulus regions in combination with state‐of‐the‐art aerosol reanalysis from Modern‐Era Retrospective Analysis for Research and Applications version 2 (MERRA2) to diagnose how aerosols affect Nd. As in previous studies, Nd is related to sulfate mass through a power law relationship. The slope of the log‐log relationship between Nd and SO4 in maritime stratocumulus is found to be 0.31, which is similar to the range of 0.2–0.8 from previous in situ studies and remote‐sensing studies in the pristine Southern Ocean. Using preindustrial emissions models, the change in Nd between preindustrial and present day is estimated. Nd is inferred to have more than tripled in some regions. Cloud properties from Moderate Resolution Imaging Spectroradiometer (MODIS) are used to estimate the radiative forcing due to this change in Nd. The Twomey effect operating in isolation is estimated to create a radiative forcing of −0.97 ± 0.23 W m−2 relative to the preindustrial era.

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.

Abstract. A 1200×1200 km2 area of the tropical South Atlantic Ocean near Ascension Island is studied with the HadGEM climate model at convection-permitting and global resolutions for a 10-day case study period in August 2016. During the simulation period, a plume of biomass burning smoke from Africa moves into the area and mixes into the clouds. At Ascension Island, this smoke episode was the strongest of the 2016 fire season.The region of interest is simulated at 4 km resolution, with no parameterised convection scheme. The simulations are driven by, and compared to, the global model. For the first time, the UK Chemistry and Aerosol model (UKCA) is included in a regional model with prognostic aerosol number concentrations advecting in from the global model at the boundaries of the region.Fire emissions increase the total aerosol burden by a factor of 3.7 and cloud droplet number concentrations by a factor of 3, which is consistent with MODIS observations. In the regional model, the inversion height is reduced by up to 200 m when smoke is included. The smoke also affects precipitation, to an extent which depends on the model microphysics. The microphysical and dynamical changes lead to an increase in liquid water path of 60 g m−2 relative to a simulation without smoke aerosol, when averaged over the polluted period. This increase is uncertain, and smaller in the global model. It is mostly due to radiatively driven dynamical changes rather than precipitation suppression by aerosol.Over the 5-day polluted period, the smoke has substantial direct radiative effects of +11.4 W m−2 in the regional model, a semi-direct effect of −30.5 W m−2 and an indirect effect of −10.1 W m−2. Our results show that the radiative effects are sensitive to the structure of the model (global versus regional) and the parameterization of rain autoconversion. Furthermore, we simulate a liquid water path that is biased high compared to satellite observations by 22 % on average, and this leads to high estimates of the domain-averaged aerosol direct effect and the effect of the aerosol on cloud albedo. With these caveats, we simulate a large net cooling across the region, of −27.6 W m−2.