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How clouds respond to anthropogenic sulfate aerosols is one of the largest sources of uncertainty in the radiative forcing of climate over the industrial era. This uncertainty limits our ability to predict equilibrium climate sensitivity (ECS)—the equilibrium global warming following a doubling of atmospheric CO 2 . Here, we use satellite observations to quantify relationships between sulfate aerosols and low-level clouds while carefully controlling for meteorology. We then combine the relationships with estimates of the change in sulfate concentration since about 1850 to constrain the associated radiative forcing. We estimate that the cloud-mediated radiative forcing from anthropogenic sulfate aerosols is − 1.11 ± 0.43 W m −2 over the global ocean (95% confidence). This constraint implies that ECS is likely between 2.9 and 4.5 K (66% confidence). Our results indicate that aerosol forcing is less uncertain and ECS is probably larger than the ranges proposed by recent climate assessments.

The extratropical shortwave (SW) cloud feedback is primarily due to increases in extratropical liquid cloud extent and optical depth. Here, we examine the response of extratropical (35°–75°) marine cloud liquid water path (LWP) to a uniform 4-K increase in sea surface temperature (SST) in global climate models (GCMs) from phase 5 of the Coupled Model Intercomparison Project (CMIP5) and variants of the HadGEM3-GC3.1 GCM. Compositing is used to partition data into periods inside and out of cyclones. The response of extratropical LWP to a uniform SST increase and associated atmospheric response varies substantially among GCMs, but the sensitivity of LWP to cloud controlling factors (CCFs) is qualitatively similar. When all other predictors are held constant, increasing moisture flux drives an increase in LWP. Increasing SST, holding all other predictors fixed, leads to a decrease in LWP. The combinations of these changes lead to LWP, and by extension reflected SW, increasing with warming in both hemispheres. Observations predict an increase in reflected SW over oceans of 0.8–1.6 W m−2per kelvin SST increase (35°–75°N) and 1.2–1.9 W m−2per kelvin SST increase (35°–75°S). This increase in reflected SW is mainly due to increased moisture convergence into cyclones because of increasing available moisture. The efficiency at which converging moisture is converted into precipitation determines the amount of liquid cloud. Thus, cyclone precipitation processes are critical to constraining extratropical cloud feedbacks.

Cloud droplet number concentration (Nd) is of central importance to observation-based estimates of aerosol indirect effects, being used to quantify both the cloud sensitivity to aerosol and the base state of the cloud. However, the derivation of Nd from satellite data depends on a number of assumptions about the cloud and the accuracy of the retrievals of the cloud properties from which it is derived, making it prone to systematic biases. A number of sampling strategies have been proposed to address these biases by selecting the most accurate Nd retrievals in the satellite data. This work compares the impact of these strategies on the accuracy of the satellite retrieved Nd, using a selection of in situ measurements. In stratocumulus regions, the MODIS Nd retrieval is able to achieve a high precision (r2 of 0.5–0.8). This is lower in other cloud regimes but can be increased by appropriate sampling choices. Although the Nd sampling can have significant effects on the Nd climatology, it produces only a 20 % variation in the implied radiative forcing from aerosol–cloud interactions, with the choice of aerosol proxy driving the overall uncertainty. The results are summarised into recommendations for using MODIS Nd products and appropriate sampling.

Mesoscale cellular convective (MCC) clouds occur in large-scale patterns over the ocean, are prevalent in sub-tropical cloud regions and mid-latitudes, and have important radiative impacts on the climate system. On average, closed MCC clouds have higher albedos than open or disorganized MCC clouds for the same cloud fraction which suggests differences in micro- and macro-physical characteristics between MCC morphologies. Marine cold air outbreaks (MCAOs) influence the development of open MCC clouds and the transition from closed to open MCC clouds in the mid-latitudes. A MCAO index, M, combines atmospheric surface forcing and static stability and can be used to examine global MCC morphology dependencies. MCC cloud morphology occurrence is also expected to shift with sea surface temperature (SST) changes as the climate warms. Analysis of MCC identifications (derived from a neural network classifier applied to MODIS satellite collection 6 liquid water path retrievals) and ECMWF ERA5 reanalysis data shows that closed MCC cloud occurrence shifts to open or disorganized MCC within an M-SST space. Global climate models (GCMs) predict that M will change regionally in strength as SSTs increase. Based on our derived MCC-M-SST relationship in the current climate, closed MCC occurrence frequency is expected to increase with a weakening of M but decrease with an increase in SSTs. This results in a shift to cloud morphologies with lower albedos. Cloud controlling factor analysis is used to estimate the resulting low cloud morphology feedback which is found to be spatially varied and between ±0.15 W m-2 K-1. Because the morphology feedback is estimated to be positive in the extra-tropics and is not currently represented in GCMs, this implies a higher climate sensitivity than GCMs currently estimate.

The change in planetary albedo due to aerosol-cloud interactions (aci) during the industrial era is the leading source of uncertainty in inferring Earth's climate sensitivity to increased greenhouse gases from the historical record. Examining pristine environments such as the Southern Ocean (SO) helps us to understand the pre-industrial state and constrain the change in cloud brightness over the industrial period associated with aci. This study presents two methods of utilizing observations of pristine environments to examine climate models and our understanding of the pre-industrial state. First, cloud droplet number concentration (Nd) is used as an indicator of aci. Global climate models (GCMs) show that the hemispheric contrast in liquid cloud Nd between the pristine SO and the polluted Northern Hemisphere observed in the present-day can be used as a proxy for the increase in Nd from the pre-industrial. A hemispheric difference constraint developed from MODIS satellite observations indicates that pre-industrial Nd may have been higher than previously thought and provides an estimate of radiative forcing associated with aci between -1.2 and -0.6 Wm-2. Comparisons with MODIS Nd highlight significant GCM discrepancies in pristine, biologically active regions. Second, aerosol and cloud microphysical observations from a recent SO aircraft campaign are used to identify two potentially important mechanisms that are incomplete or missing in GCMs: i) production of new aerosol particles through synoptic uplift, and ii) buffering of Nd against precipitation removal by small, Aitken mode aerosols entrained from the free troposphere. The latter may significantly contribute to the high, summertime SO Nd levels which persist despite precipitation depletion associated with mid-latitude storm systems. Observational comparisons with nudged Community Atmosphere Model version 6 (CAM6) hindcasts show low-biased SO Nd is linked to under-production of free-tropospheric Aitken aerosol which drives low-biases in cloud condensation nuclei number and likely discrepancies in composition. These results have important implications for the ability of current GCMs to capture aci in pristine environments.

Significance Enhancement of aerosol that can nucleate cloud droplets increases the droplet number concentration and albedo of clouds. This increases the amount of sunlight reflected to space. Uncertainty in how aerosol−cloud interactions over the industrial period have increased planetary albedo by this mechanism leads to significant uncertainty in climate projections. Our work presents a method for observationally constraining the change in albedo due to anthropogenic aerosol emissions: a hemispheric difference in remotely sensed cloud droplet number between the pristine Southern Ocean (a preindustrial proxy) and the polluted Northern Hemisphere. Application of this constraint to climate models reduces the range of estimated albedo change since industrialization and suggests current models underpredict cloud droplet number concentration in the preindustrial era., The change in planetary albedo due to aerosol−cloud interactions during the industrial era is the leading source of uncertainty in inferring Earth’s climate sensitivity to increased greenhouse gases from the historical record. The variable that controls aerosol−cloud interactions in warm clouds is droplet number concentration. Global climate models demonstrate that the present-day hemispheric contrast in cloud droplet number concentration between the pristine Southern Hemisphere and the polluted Northern Hemisphere oceans can be used as a proxy for anthropogenically driven change in cloud droplet number concentration. Remotely sensed estimates constrain this change in droplet number concentration to be between 8 cm−3 and 24 cm−3. By extension, the radiative forcing since 1850 from aerosol−cloud interactions is constrained to be −1.2 W⋅m−2 to −0.6 W⋅m−2. The robustness of this constraint depends upon the assumption that pristine Southern Ocean droplet number concentration is a suitable proxy for preindustrial concentrations. Droplet number concentrations calculated from satellite data over the Southern Ocean are high in austral summer. Near Antarctica, they reach values typical of Northern Hemisphere polluted outflows. These concentrations are found to agree with several in situ datasets. In contrast, climate models show systematic underpredictions of cloud droplet number concentration across the Southern Ocean. Near Antarctica, where precipitation sinks of aerosol are small, the underestimation by climate models is particularly large. This motivates the need for detailed process studies of aerosol production and aerosol−cloud interactions in pristine environments. The hemispheric difference in satellite estimated cloud droplet number concentration implies preindustrial aerosol concentrations were higher than estimated by most models.

Global climate models (GCMs) differ greatly in their shortwave cloud feedback. One feature that is consistent across GCMs is a positive shortwave cloud feedback in the subtropics, and a negative shortwave cloud feedback across the midlatitudes. Confidence has grown in the mechanisms that lead to, and the strength of, the subtropical shortwave cloud feedback, but the midlatitude negative shortwave cloud feedback is not well-constrained or well-understood. It is critical to reduce uncertainty in midlatitude shortwave cloud feedback. A more positive midlatitude shortwave cloud feedback in the sixth coupled model intercomparison project (CMIP6) has been found to be one of the primary causes of the increased climate sensitivity of CMIP6 models relative to CMIP5. We show that changes in midlatitude cyclones in future climates are the primary cause of the negative shortwave cloud feedback and are thus key to understanding the high climate sensitivity in the most recent GCMs. Warming-induced changes in cloud liquid water path in midlatitude cyclones can almost entirely be explained by Clausius-Clapeyron increasing moisture convergence into cyclones. One concern with simulating midlatitude cyclones is the lack of predictive skill at low resolution. A more realistic relationship between moisture flux and cyclone liquid content is found at high horizontal resolution (∆x Predicted midlatitude cloud feedbacks based on convection-permitting model output (model output is shown in a). The moisture flux along the warm conveyor belt (WCB) of a cyclone plays a central role in determining cyclone cloud liquid water path (LWP) (b). Because WCB scales with water vapor path (WVP) and surface wind speed, WCB moisture flux increases following Clausius-Clapeyron and predicts a negative midlatitude cloud feedback.

Equilibrium climate sensitivity, the global surface temperature response to CO urn:x-wiley:grl:media:grl60047:grl60047-math-0001 doubling, has been persistently uncertain. Recent consensus places it likely within 1.5–4.5 K. Global climate models (GCMs), which attempt to represent all relevant physical processes, provide the most direct means of estimating climate sensitivity via CO urn:x-wiley:grl:media:grl60047:grl60047-math-0002 quadrupling experiments. Here we show that the closely related effective climate sensitivity has increased substantially in Coupled Model Intercomparison Project phase 6 (CMIP6), with values spanning 1.8–5.6 K across 27 GCMs and exceeding 4.5 K in 10 of them. This (statistically insignificant) increase is primarily due to stronger positive cloud feedbacks from decreasing extratropical low cloud coverage and albedo. Both of these are tied to the physical representation of clouds which in CMIP6 models lead to weaker responses of extratropical low cloud cover and water content to unforced variations in surface temperature. Establishing the plausibility of these higher sensitivity models is imperative given their implied societal ramifications.

Representing large-scale co-variability between variables related to aerosols, clouds and radiation is one of many aspects of agreement with observations desirable for a climate model. In this study such relations are investigated in terms of temporal correlations on monthly mean scale, to identify points of agreement and disagreement with observations. Ten regions with different meteorological characteristics and aerosol signatures are studied and correlation matrices for the selected regions offer an overview of model ability to represent present day climate variability. Global climate models with different levels of detail and sophistication in their representation of aerosols and clouds are compared with satellite observations and reanalysis assimilating meteorological fields as well as aerosol optical depth from observations. One example of how the correlation comparison can guide model evaluation and development is the often studied relation between cloud droplet number and water content. Reanalysis, with no parameterized aerosol–cloud coupling, shows weaker correlations than observations, indicating that microphysical couplings between cloud droplet number and water content are not negligible for the co-variations emerging on larger scale. These observed correlations are, however, not in agreement with those expected from dominance of the underlying microphysical aerosol–cloud couplings. For instance, negative correlations in subtropical stratocumulus regions show that suppression of precipitation and subsequent increase in water content due to aerosol is not a dominating process on this scale. Only in one of the studied models are cloud dynamics able to overcome the parameterized dependence of rain formation on droplet number concentration, and negative correlations in the stratocumulus regions are reproduced.

Decreases in subtropical low cloud cover (LCC) occur in climate model simulations of global warming. In this study 8-day-averaged observations from the Moderate Resolution Imaging Spectroradiometer (MODIS) and the Atmospheric Infrared Sounder (AIRS) spanning 2002–14 are combined with European Centre for Medium-Range Weather Forecasts (ECMWF) interim reanalysis to compute the dependence of the observed variability of LCC on various predictor variables. Large-scale thermodynamic and dynamic predictors of LCC are selected based on insight from large-eddy simulations (LESs) and observational analysis. It is found that increased estimated inversion strength (EIS) is associated with increased LCC. Drying of the free troposphere is associated with decreased LCC. Decreased LCC accompanies subsidence in regions of relatively low EIS; the opposite is found in regions of high EIS. Finally, it is found that increasing sea surface temperature (SST) leads to a decrease in LCC. These results are in keeping with previous studies of monthly and annual data. Based upon the observed response of LCC to natural variability of the control parameters, the change in LCC is estimated for an idealized warming scenario where SST increases by 1 K and EIS increases by 0.2 K. For this change in EIS and SST the LCC is inferred to decrease by 0.5%–2.7% when the regression models are trained on data observed between 40°S and 40°N and by 1.1%–1.4% when trained on data from trade cumulus–dominated regions. When the data used to train the regression model are restricted to stratocumulus-dominated regions the change in LCC is highly uncertain and varies between −1.6% and +1.4%, depending on the stratocumulus-dominated region used to train the regression model.

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 fr ...

Aerosol-cloud interactions represent the leading uncertainty in our ability to infer climate sensitivity from the observational record. The forcing from changes in cloud albedo driven by increases in cloud droplet number (Nd) (the first indirect effect) is confidently negative and has narrowed its probable range in the last decade, but the sign and strength of forcing associated with changes in cloud macrophysics in response to aerosol (aerosol-cloud adjustments) remain uncertain. This uncertainty reflects our inability to accurately quantify variability not associated with a causal link flowing from the cloud microphysical state to cloud macrophysical state. Once variability associated with meteorology has been removed, covariance between the liquid water path averaged across cloudy and clear regions (LWP, here, characterizing the macrophysical state) and Nd (characterizing the microphysical) is the sum of two causal pathways linking Nd to LWP: Nd altering LWP (adjustments) and precipitation scavenging aerosol and thus depleting Nd. Only the former term is relevant to constraining adjustments, but disentangling these terms in observations is challenging. We hypothesize that the diversity of constraints on aerosol-cloud adjustments in the literature may be partly due to not explicitly characterizing covariance flowing from cloud to aerosol, and aerosol to cloud. Here, we restrict our analysis to the regime of extratropical clouds outside of low-pressure centers associated with cyclonic activity. Observations from MAC-LWP, and MODIS are compared to simulations in the MetOffice Unified Model (UM) GA7.1 (the atmosphere model of HadGEM3-GC3.1 and UKESM1). The meteorological predictors of LWP are found to be similar between the model and observations. There is also agreement with previous literature on cloud-controlling factors finding that increasing stability, moisture, and sensible heat flux enhance LWP, while increasing subsidence, and sea surface temperature decrease it. A simulation where cloud microphysics are insensitive to changes in Nd is used to characterize covariance between Nd and LWP that is induced by factors other than aerosol-cloud adjustments. By removing variability associated with meteorology and scavenging we infer the sensitivity of LWP to changes in Nd. Application of this technique to UM GA7.1 simulations reproduces the true model adjustment strength. Observational constraints developed using simulated covariability not induced by adjustments and observed covariability between Nd and LWP predict a 25–30 % overestimate by the UM GA7.1 in LWP change and a 30–35% overestimate in associated radiative forcing.

A negative extratropical shortwave cloud feedback driven by changes in cloud optical depth is a feature of global climate models (GCMs). A robust positive trend in observed liquid water path (LWP) over the last two decades across the warming Southern Ocean supports the negative shortwave cloud feedback predicted by GCMs. This feature has been proposed to be due to transitions from ice to liquid with warming. To gain insight into the shortwave cloud feedback we examine extratropical cyclone variability and the response of extratropical cyclones to transient warming in GCM simulations. Multi-Sensor Advanced Climatology Liquid Water Path (MAC-LWP) microwave observations of cyclone properties from the period 1992–2015 are contrasted with GCM simulations, with horizontal resolutions ranging from 7 km to hundreds of kilometers. We find that inter-cyclone variability in LWP in both observations and models is strongly driven by the moisture flux along the cyclone's warm conveyor belt (WCB). Stronger WCB moisture flux enhances the LWP within cyclones. This relationship is replicated in GCMs, although its strength varies substantially across models. It is found that more than 80 % of the enhancement in Southern Hemisphere (SH) extratropical cyclone LWP in GCMs in response to a transient 4 K warming can be predicted based on the relationship between the WCB moisture flux and cyclone LWP in the historical climate and their change in moisture flux between the historical and warmed climates. Further, it is found that that the robust trend in cyclone LWP over the Southern Ocean in observations and GCMs is consistent with changes in the moisture flux. We propose two cloud feedbacks acting within extratropical cyclones: a negative feedback driven by Clausius–Clapeyron increasing water vapor path (WVP), which enhances the amount of water vapor available to be fluxed into the cyclone, and a feedback moderated by changes in the life cycle and vorticity of cyclones under warming, which changes the rate at which existing moisture is imported into the cyclone. Both terms contribute to increasing LWP within the cyclone. While changes in moisture flux predict cyclone LWP trends in the current climate and the majority of changes in LWP in transient warming simulations, a portion of the LWP increase in response to climate change that is unexplained by increasing moisture fluxes may be due to phase transitions. The variability in LWP within cyclone composites is examined to understand what cyclonic regimes the mixed-phase cloud feedback is relevant to. At a fixed WCB moisture flux cyclone LWP increases with increasing sea surface temperature (SST) in the half of the composite poleward of the low and decreases in the half equatorward of the low in both GCMs and observations. Cloud-top phase partitioning observed by the Atmospheric Infrared Sounder (AIRS) indicates that phase transitions may be driving increases in LWP in the poleward half of cyclones.

In this study, it is shown that CMIP5 global climate models (GCMs) that convert supercooled water to ice at relatively warm temperatures tend to have a greater mean-state cloud fraction and more negative cloud feedback in the middle and high latitude Southern Hemisphere. We investigate possible reasons for these relationships by analyzing the mixed-phase parameterizations in 26 GCMs. The atmospheric temperature where ice and liquid are equally prevalent (T5050) is used to characterize the mixed-phase parameterization in each GCM. Liquid clouds have a higher albedo than ice clouds, so, all else being equal, models with more supercooled liquid water would also have a higher planetary albedo. The lower cloud fraction in these models compensates the higher cloud reflectivity and results in clouds that reflect shortwave radiation (SW) in reasonable agreement with observations, but gives clouds that are too bright and too few. The temperature at which supercooled liquid can remain unfrozen is strongly anti-correlated with cloud fraction in the climate mean state across the model ensemble, but we know of no robust physical mechanism to explain this behavior, especially because this anti-correlation extends through the subtropics. A set of perturbed physics simulations with the Community Atmospheric Model Version 4 (CAM4) shows that, if its temperature-dependent phase partitioning is varied and the critical relative humidity for cloud formation in each model run is also tuned to bring reflected SW into agreement with observations, then cloud fraction increases and liquid water path (LWP) decreases with T5050, as in the CMIP5 ensemble.

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.

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., Key Points Satellite cloud droplet concentration uncertainties of 78% for pixel‐level retrievals and 54% for 1 by 1 degree retrievals are estimatedThe effective radius retrieval is the most important aspect for improvement, and more in situ evaluation is neededPotential improvements using passive and active satellite, and ground‐based instruments are discussed

This chapter introduces cloud feedbacks and describes salient features of their structure. One particularly pronounced feature simulated by global climate models (GCMs), is the contrast between the subtropics where cloud cover decreases with warming (a positive feedback) and the mid- and high-latitudes where cloud albedo increases with warming (a negative feedback). This increase in cloud albedo appears to be due to mixed-phase clouds (MPCs) transitioning from a more ice-dominated to more liquid-dominated state. The representation of this behavior in GCMs is discussed and is compared to satellite observations. Observational constraints on the MPC feedback show that the current generation of GCMs have too strong an increase in planetary albedo due to ice transitioning to liquid in the mid- and high-latitudes, indicating a potential underestimation of climate sensitivity. This behavior appears to be at least partially due to an inability to maintain supercooled liquid water at sufficiently low temperatures.

The sensitivity of the reflection of shortwave radiation over the Southern Ocean to the cloud properties there is estimated using observations from a suite of passive and active satellite instruments in combination with radiative transfer modeling. A composite cloud property observational data description is constructed that consistently incorporates mean cloud liquid water content, ice water content, liquid and ice particle radius information, vertical structure, vertical overlap, and spatial aggregation of cloud water as measured by optical depth versus cloud-top pressure histograms. The observational datasets used are Moderate Resolution Imaging Spectroradiometer (MODIS) effective radius filtered to mitigate solar zenith angle bias, the Multiangle Imaging Spectroradiometer (MISR) cloud-top height–optical depth (CTH–OD) histogram, the liquid water path from the University of Wisconsin dataset, and ice cloud properties from CloudSat. This cloud database is used to compute reflected shortwave radiation as a function of month and location over the ocean from 40° to 60°S, which compares well with observations of reflected shortwave radiation. This calculation is then used to test the sensitivity of the seasonal variation of shortwave reflection to the observed seasonal variation of cloud properties. Effective radius decreases during the summer season, which results in an increase in reflected solar radiation of 4–8 W m−2 during summer compared to what would be reflected if the effective radius remained constant at its annual-mean value. Summertime increases in low cloud fraction similarly increase the summertime reflection of solar radiation by 9–11 W m−2. In-cloud liquid water path is less in summertime, causing the reflected solar radiation to be 1–4 W m−2 less.

Climate models produce an increase in cloud optical depth in midlatitudes associated with climate warming, but the magnitude of this increase and its impact on reflected solar radiation vary from model to model. Transition from ice to liquid in midlatitude clouds is thought to be one mechanism for producing increased cloud optical depth. Here observations of cloud properties are used from a suite of remote sensing instruments to estimate the effect of conversion of ice to liquid associated with warming on reflected solar radiation in the latitude band from 40° to 60°S. The calculated increase in upwelling shortwave radiation (SW↑) is found to be important and of comparable magnitude to the increase in SW↑ associated with warming-induced increases of optical depth in climate models. The region where the authors' estimate increases SW↑ extends farther equatorward than the region where optical depth increases with warming in models. This difference is likely caused by other mechanisms at work in the models but is also sensitive to the amount of ice present in climate models and its susceptibility to warming.

Aerosol-cloud interactions are a major source of uncertainty in predicting 21st century climate change. Using high-resolution, convection-permitting global simulations we predict that increased cloud condensation nuclei (CCN) interacting with midlatitude cyclones will increase their cloud droplet number concentration (CDNC), liquid water (CLWP), and albedo. For the first time this effect is shown with 13 years of satellite observations. Causality between enhanced CCN and enhanced cyclone liquid content is supported by the 2014 eruption of Holuhraun. The change in midlatitude cyclone albedo due to enhanced CCN in a surrogate climate model is around 70 % of the change in a high-resolution convection-permitting model, indicating that climate models may underestimate this indirect effect.

Exploiting the observed robust relationships between temperature and optical depth in extratropical clouds, we calculate the shortwave cloud feedback from historical data, by regressing observed and modeled cloud property histograms onto local temperature in middle to high southern latitudes. In this region, all CMIP5 models and observational data sets predict a negative cloud feedback, mainly driven by optical thickening. Between 45° and 60°S, the mean observed shortwave feedback (−0.91 ± 0.82 W m−2 K−1, relative to local rather than global mean warming) is very close to the multimodel mean feedback in RCP8.5 (−0.98 W m−2 K−1), despite differences in the meridional structure. In models, historical temperature-cloud property relationships reliably predict the forced RCP8.5 response. Because simple theory predicts this optical thickening with warming, and cloud amount changes are relatively small, we conclude that the shortwave cloud feedback is very likely negative in the real world at middle to high latitudes.

The Barðarbunga-Veiðivotn fissure eruption lasted from 31 August 2014 to 28 February 2015, during which its sulfur emissions dwarfed anthropogenic emissions from Europe. This natural experiment offers an excellent opportunity to investigate the aerosol indirect effect and the effect of effusive volcanic eruptions on climate. During the eruption cloud droplet effective radius (re) over the region surrounding Iceland was at the lowest value in the 14 year Moderate Imaging Spectroradiometer data record during September and October 2014. The change in reflected solar radiation due to increased cloud reflectivity during September and October is estimated to exceed 2 W m−2 over the region surrounding Iceland, with increases of 1 W m−2 extending as far south as the Acores. The strength of the aerosol indirect effect diagnosed here reaffirms the ability of volcanic aerosols to affect cloud properties and ultimately the planetary albedo.

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.

Sulfate and organic mass in sea spray explain more than half of the variability in Southern Ocean cloud droplet concentration., Atmospheric aerosols, suspended solid and liquid particles, act as nucleation sites for cloud drop formation, affecting clouds and cloud properties—ultimately influencing the cloud dynamics, lifetime, water path, and areal extent that determine the reflectivity (albedo) of clouds. The concentration Nd of droplets in clouds that influences planetary albedo is sensitive to the availability of aerosol particles on which the droplets form. Natural aerosol concentrations affect not only cloud properties themselves but also modulate the sensitivity of clouds to changes in anthropogenic aerosols. It is shown that modeled natural aerosols, principally marine biogenic primary and secondary aerosol sources, explain more than half of the spatiotemporal variability in satellite-observed Nd. Enhanced Nd is spatially correlated with regions of high chlorophyll a, and the spatiotemporal variability in Nd is found to be driven primarily by high concentrations of sulfate aerosol at lower Southern Ocean latitudes (35o to 45oS) and by organic matter in sea spray aerosol at higher latitudes (45o to 55oS). Biogenic sources are estimated to increase the summertime mean reflected solar radiation in excess of 10 W m–2 over parts of the Southern Ocean, which is comparable to the annual mean increases expected from anthropogenic aerosols over heavily polluted regions of the Northern Hemisphere.

Dynamical properties of short freely jointed and freely rotating chains are studied using molecular dynamics simulations. These results are combined with those of previous studies, and the degree of rheological complexity of the two models is assessed. New results are based on an improved analysis procedure of the rotational relaxation of the second Legendre polynomials of the end-to-end vector in terms of the Kohlrausch-Williams-Watts (KWW) function. Increased accuracy permits the variation of the KWW stretching exponent beta to be tracked over a wide range of state points. The smoothness of beta as a function of packing fraction eta is a testimony both to the accuracy of the analytical methods and the appropriateness of (eta(0)-eta) as a measure of the distance to the ideal glass transition at eta(0). Relatively direct comparison is made with experiment by viewing beta as a function of the KWW relaxation time tau(KWW). The simulation results are found to be typical of small molecular glass formers. Several manifestations of rheological complexity are considered. First, the proportionality of alpha-relaxation times is explored by the comparison of translational to rotational motion (i.e., the Debye-Stokes-Einstein relation), of motion on different length scales (i.e., the Stokes-Einstein relation), and of rotational motion at intermediate times to that at long time. Second, the range of time-temperature superposition master curve behavior is assessed. Third, the variation of beta across state points is tracked. Although no particulate model of a liquid is rigorously rheologically simple, we find freely jointed chains closely approximated this idealization, while freely rotating chains display distinctly complex dynamical features.