Engineering Papers⌕ Search

SEARCH · Engineering Papers

Results for “cloud radiative effects”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 109 records · Page 6

Reducing Southern Ocean Shortwave Radiation Errors in the ERA5 Reanalysis with Machine Learning and 25 Years of Surface Observations

Earth system models struggle to simulate clouds and their radiative effects over the Southern Ocean, partly due to a lack of measurements and targeted cloud microphysics knowledge. We have evaluated biases of downwelling shortwave radiation in the ERA5 climate reanalysis using 25 years (1995–2019) of summertime surface measurements, collected on the Research and Supply Vessel (RSV) Aurora Australis, the Research Vessel (R/V) Investigator, and at Macquarie Island. During October–March daylight hours, the ERA5 simulation of SW down exhibited large errors (mean bias = 54 W m -2 , mean absolute error = 82 W m -2 , root-mean-square error = 132 W m -2 , and R 2 = 0.71). To determine whether we could improve these statistics, we bypassed ERA5’s radiative transfer model for SW down with machine learning–based models using a number of ERA5’s gridscale meteorological variables as predictors. These models were trained and tested with the surface measurements of SW down using a 10-fold shuffle split. An extreme gradient boosting (XGBoost) and a random forest–based model setup had the best performance relative to ERA5, both with a near complete reduction of the mean bias error, a decrease in the mean absolute error and root-mean-square error by 25% ± 3%, and an increase in the R 2 value of 5% ± 1% over the 10 splits. Large improvements occurred at higher latitudes and cyclone cold sectors, where ERA5 performed most poorly. We further interpret our methods using Shapley additive explanations. Our results indicate that data-driven techniques could have an important role in simulating surface radiation fluxes and in improving reanalysis products.

54 ENVIRONMENTAL SCIENCES↗

Enhanced Cloud Top Longwave Radiative Cooling Due To the Effect of Horizontal Radiative Transfer in the Stratocumulus to Trade Cumulus Transition Regime

Abstract Recent studies develop the SPeedy Algorithm for Radiative TrAnsfer through CloUd Sides (SPARTACUS) to handle the influence of horizontal RT on vertical radiative fluxes within an atmospheric column. The present study applies SPARTACUS to large eddy simulation (LES)‐generated cloud fields across the stratocumulus to trade cumulus transition (STCT) regime with coarse and fine vertical resolutions. The results show that, as the vertical resolution increases, radiation simulations show increasingly stronger cloud‐top longwave (LW) radiative cooling. Consequently, the sharp radiative heating gradient across the cloud layer in the LES‐like resolution simulations cannot be resolved with the coarse resolution simulations. Including the horizontal RT typically enhances cloud LW radiative cooling rate by less than 10% for all the cloud fields but more significantly in the cloud fields during the STCT. The enhanced cloud LW radiative cooling also occurs in the lower cloud layer in the decoupled cumulus cloud regime.

Geology↗

Using Downwelling Far- and Thermal-Infrared Hyperspectral Radiance for Cloud Phase Classification in the Antarctic

The cloud phase is one of the most important parameters of clouds. In this paper, we propose a method for cloud phase classification that synergistically utilizes the far- and thermal-infrared bands based on the Atmospheric Emitted Radiance Interferometer (AERI) at the Atmospheric Radiation Measurement West Antarctic Radiation Experiment (AWARE) observatory in 2016. The possible features in the far- and thermal-infrared bands are analyzed based on the differences in the simulated cloud brightness temperature (BT) spectra with different cloud phases. Using the support vector machine (SVM) algorithm, four features are determined to identify the cloud phase, which include the BT at 900 cm -1 , the slope of the fitted function of BT in the 900–1000 cm -1 interval, the BT difference (BTD) between 512 cm -1 and 726 cm -1 , and the BTD between 550 cm -1 and 726 cm -1 . Here, the performance of the proposed method is evaluated with Shupe’s and Turner’s method. The monthly average accuracy of the proposed method, the method without the two far-infrared features, and Turner’s method are about 76%, 36%, and 49%, respectively, which infer the good performance of the proposed method and also indicate that the far-infrared band features can effectively enhance cloud phase classification. It is notable that, compared to Shupe’s method, the accuracy for the proposed method is only 61% during the Antarctic summer, which results from the definitions of cloud phase and radiative effect. In addition, the accuracy is only 44% for Turner’s method in seasons with a low frequency of mixed clouds due to the significant effect of water vapor.

54 ENVIRONMENTAL SCIENCES↗

Dust semi-direct effects: low-level cloud response to free-tropospheric dust-induced longwave radiation over the North Atlantic Ocean

Aerosol semi-direct effect is the adjustment of the radiative budget due to the cloud response to radiation absorption. Although dust accounts for about a third of aerosols' shortwave absorption, our understanding of its semi-direct effect often relies on traditional shortwave-focused mechanisms previously established for biomass-burning aerosols, and implications of dust longwave absorption on clouds have yet to be explored. Here, we assess the low-level cloud cover (LLCC) response to changes in properties and characteristics of the free-tropospheric dust layer over the North Atlantic Ocean (May–August, 2007–2017). We find that, consistent with previous studies, LLCC typically responds positively (increases in clouds) to an overlying dust layer. However, this response weakens with increasing dust optical depth (DOD), dust geometric thickness (DGT), and dust-layer base height (DBH). Specifically, we find that the LLCC response weakens by 4.3 ± 1.04 % and 1.6 ± 0.65 %, respectively, for a one-standard-deviation increase in DOD and DGT, and a smaller response to DBH (0.19 ± 0.45 %). We also find that the weakened LLCC response is primarily due to enhanced dust-induced longwave-dominated cloud-top warming, which counteracts the mean cloud-top cooling by as much as 19 % (mean of 9 %). Sensitivity analysis further indicates that the variability in dust properties, influenced by dust size distribution and refractive index, dominates the changes in dust-induced cloud-top warming, rather than variabilities in cloud properties or thermodynamic profiles. Our result adds to the traditional understanding of LLCC enhancement through shortwave-driven atmospheric stability, often associated with aerosol semi-direct effects, and highlights the role of dust-induced cloud-top longwave warming in dust semi-direct effects.

Pandey, Satyendra K. [Univ. of California, Merced,↗

The Interaction Between Climate Forcing and Feedbacks

A Perturbed Parameter Ensemble (PPE) with the Community Atmosphere Model version 6 (CAM6) is used to better understand the sensitivity of aerosol forcing and cloud feedbacks to changes in model processes. Aerosol forcing through aerosol-cloud interactions is mostly negative (a cooling) due to shortwave radiation, while feedbacks are positive or negative in different regions due to contrasting longwave and shortwave effects. Both forcing and feedbacks are related to the mean climate state. Higher magnitude cloud radiative effects generally mean larger magnitude net negative forcing and larger magnitude net positive feedback. Aerosol forcing is broadly related to the susceptibility of clouds to drop number. Feedbacks also related to susceptibility, but to a lesser extent and in different regions to aerosol forcing. Aerosol forcing and cloud feedbacks are anti-correlated in the CAM6 PPE such that stronger negative forcing is associated with stronger positive feedbacks. Even the processes governing forcing and feedback sensitivity in the PPE are similar. These include the warm rain formation process, ice loss processes and deep convective intensity.

54 ENVIRONMENTAL SCIENCES↗

Performance of Cloud 3D Solvers in Ice Cloud Shortwave Radiation Closure Over the Equatorial Western Pacific Ocean

Abstract For retrieving cloud optical properties from satellite images or computing these properties from climate model output, computationally efficient treatments of cloud horizontal inhomogeneity include the Monte Carlo Independent Column Approximation (McICA) and the Tripleclouds method. Computationally efficient treatment of cloud horizontal radiation exchanges includes the SPeedy Algorithm for Radiative TrAnsfer through CloUd Sides (SPARTACUS). As a test to derive properties from satellite images, we collocate Moderate Resolution Imaging Spectroradiometer (MODIS) cloud retrievals with near‐nadir Cloud and the Earth's Radiant Energy System (CERES) footprints in July 2008 over an equatorial western Pacific Ocean region to compare the performance of the McICA, Tripleclouds, and SPARTACUS solvers to the conventional plane‐parallel homogeneous (PPH) treatment. PPH overestimates cloud albedo, and the three solvers effectively reduce overestimation with root mean square error of shortwave upwelling irradiance decreasing between 15.72 and 18.53 W m −2 , or about 22%–25%. Although cloud top variability does not get fed into the simulations, all three solvers also reduce the effect of cloud top variability on cloud albedo. Entrapment (energy reflected downward from clouds) and horizontal radiation transfer have opposite effects on the SPARTACUS cloud albedo simulation. The net effect depends on the cloud vertical extent, the unawareness of which limits the performance of the SPARTACUS solver.

54 ENVIRONMENTAL SCIENCES↗

Implementation and Evaluation of Physics-Driven Dynamic Entrainment-Mixing Parameterization in a Climate Model and Its Impact on Low-Cloud Simulation

The turbulent entrainment-mixing process in the Community Earth System Model version 1.2 (CESM1.2) is assumed to follow the extremely inhomogeneous entrainment-mixing. However, different entrainment-mixing scenarios can occur in real clouds. To address this deficiency, a unifying parameterization that represents different entrainment-mixing processes is implemented and evaluated in CESM1.2. The results indicate that the homogeneous mixing degree values simulated by the new parameterization in CESM1.2 are predominantly greater than 50%, suggesting a tendency toward homogeneous mixing. Compared to the extremely inhomogeneous mixing mechanism, the new parameterization increases the cloud droplet number concentration (Nc). More importantly, the new parameterization improves low-cloud fraction (CLDLOW) simulation in Northwest Pacific (NWP) and Southeast Pacific (SEP) regions, with relative improvements of 2.95% and 4.17%, respectively. Furthermore, the improvements reach up to 44.6% and 16.2% in the NWP and SEP regions, respectively, when considering the relationship between N c and CLDLOW. Further analysis reveals that the new parameterization enhances cloud optical depth, longwave radiative cooling effect, net condensation rate, cloud water mixing ratio, lower-troposphere stability, and CLDLOW by increasing N c . Additionally, these results underscore the importance of improving entrainment-mixing parameterization in climate models.

54 ENVIRONMENTAL SCIENCES↗

Process‐Oriented Calibration of a Turbulence Scheme in the DOE's Global Storm‐Resolving Model Using Machine Learning

A process‐oriented calibration framework is developed for the Simplified Higher‐Order Closure (SHOC) turbulence scheme in DOE's Simple Cloud Resolving E3SM Atmospheric Model (SCREAM). This framework leverages machine learning surrogates and observational constraints to efficiently calibrate SHOC adjustable parameters across two convective regimes: clear‐sky dry convective boundary layer and fair‐weather shallow cumulus clouds from ARM observations. We use perturbed‐parameter ensembles of a doubly periodic version of SCREAM to train surrogates and apply Markov Chain Monte Carlo sampling guided by cost functions based on benchmarking large‐eddy simulations and observations to identify optimized parameter sets that perform well in both regimes. The calibrated SHOC parameters substantially improve boundary‐layer turbulence and cloud boundaries, and modeled cloud fraction and radiative effects align better with observations than the default. These results demonstrate that combining multiple process‐specific convective regimes with machine‐learning surrogates can reduce parametric uncertainties and yield a model more faithful to cloud–turbulence interactions.

58 GEOSCIENCES↗

Isolating the effect of biomass burning aerosol emissions on 20th century hydroclimate in South America and Southeast Asia

Abstract Biomass burning is a significant source of aerosol emissions in some regions and has a considerable impact on regional climate. Earth system model simulations indicate that increased biomass burning aerosol emissions contributed to statistically significant decreases in tropical precipitation over the 20th century. In this study, we use the Community Earth System Model version 1 Large Ensemble (CESM1-LENS) experiment to evaluate the mechanisms by which biomass burning aerosol contributed to decreased tropical precipitation, with a focus on South America and Southeast Asia. We analyze the all-but-one forcing simulations in which biomass burning aerosol emissions are held constant while other forcings (e.g., greenhouse gas concentrations) vary throughout the 20th century. This allows us to isolate the influence of biomass burning aerosol on processes that contribute to decreasing precipitation, including cloud microphysics, the radiative effects of absorbing aerosol particles, and alterations in regional circulation. We also show that the 20th century reduction in precipitation identified in the CESM1-LENS historical and biomass burning experiments is consistent across Coupled Model Intercomparison Project Phase 5 models with interactive aerosol schemes and the CESM2 single-forcing experiment. Our results demonstrate that higher concentrations of biomass burning aerosol increases the quantity of cloud condensation nuclei and cloud droplets, limiting cloud droplet size and precipitation formation. Additionally, absorbing aerosols (e.g., black carbon) contribute to a warmer cloud layer, which promotes cloud evaporation, increases atmospheric stability, and alters regional circulation patterns. Corresponding convectively coupled circulation responses, particularly over the tropical Andes, contribute to further reducing the flow of moisture and moisture convergence over tropical land. These results elucidate the processes that affect the water cycle in regions prone to biomass burning and inform our understanding of how future changes in aerosol emissions may impact tropical precipitation over the 21st century.

Environmental Sciences & Ecology↗

Improving vertical detail in simulated temperature and humidity data using machine learning

Atmospheric models used for weather forecasting and climate predictions discretise the atmosphere onto a vertical grid. There are however atmospheric phenomena that occur on scales smaller than the thickness of those model layers. The formation of low-level clouds due to temperature inversions is an example. This leads to atmospheric models underestimating, or even missing, these clouds and their radiative effects. Using radiosonde observations as training data, a machine learning model is used to improve the vertical detail of modelled profiles of temperature and specific humidity. In addition, a physics-informed machine learning model is developed and compared to the traditional approach; showing improvements in the cloud fraction profiles calculated from its predictions. The vertically enhanced profiles also improve the representation of layers of convective inhibition and anomalous refractivity gradients. This work facilitates targeted improvements to the representation of certain atmospheric processes without the burden of increased memory and computational cost from increasing vertical resolution throughout the whole model.

54 ENVIRONMENTAL SCIENCES↗

A central arctic extreme aerosol event triggered by a warm air-mass intrusion

Frequency and intensity of warm and moist air-mass intrusions into the Arctic have increased over the past decades and have been related to sea ice melt. During our year-long expedition in the remote central Arctic Ocean, a record-breaking increase in temperature, moisture and downwelling-longwave radiation was observed in mid-April 2020, during an air-mass intrusion carrying air pollutants from northern Eurasia. The two-day intrusion, caused drastic changes in the aerosol size distribution, chemical composition and particle hygroscopicity. Here we show how the intrusion transformed the Arctic from a remote low-particle environment to an area comparable to a central-European urban setting. Additionally, the intrusion resulted in an explosive increase in cloud condensation nuclei, which can have direct effects on Arctic clouds’ radiation, their precipitation patterns, and their lifetime. Thus, unless prompt actions to significantly reduce emissions in the source regions are taken, such intrusion events are expected to continue to affect the Arctic climate.

54 ENVIRONMENTAL SCIENCES↗

Exploring the elevated water vapor signal associated with the free tropospheric biomass burning plume over the southeast Atlantic Ocean

In southern Africa, widespread agricultural fires produce substantial biomass burning (BB) emissions over the region. The seasonal smoke plumes associated with these emissions are then advected westward over the persistent stratocumulus cloud deck in the southeast Atlantic (SEA) Ocean, resulting in aerosol effects which vary with time and location. Much work has focused on the effects of these aerosol plumes, but previous studies have also described an elevated free tropospheric water vapor signal over the SEA. Water vapor influences climate in its own right, and it is especially important to consider atmospheric water vapor when quantifying aerosol-cloud interactions and aerosol radiative effects. Here we present airborne observations made during the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) campaign over the SEA Ocean. In observations collected from multiple independent instruments on the NASA P-3 aircraft (from near-surface to 6-7 km), we observe a strongly linear correlation between pollution indicators (carbon monoxide (CO) and aerosol loading) and atmospheric water vapor content, seen at all altitudes above the boundary layer. The focus of the current study is on the especially strong correlation observed during the ORACLES-2016 deployment (out of Walvis Bay, Namibia), but a similar relationship is also observed in the August 2017 and October 2018 ORACLES deployments. Using reanalyses from the European Centre for Medium-Range Weather Forecasts (ECMWF) and Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2), and specialized WRF-Chem simulations, we trace the plume-vapor relationship to an initial humid, smoky continental source region, where it mixes with clean, dry upper tropospheric air and then is subjected to conditions of strong westward advection, namely the southern African easterly jet (AEJ-S). Our analysis indicates that air masses likely left the continent with the same relationship between water vapor and carbon monoxide as was observed by aircraft. This linear relationship developed over the continent due to daytime convection within a deep continental boundary layer (up to ~5-6 km) and mixing with higher-altitude air, which resulted in fairly consistent vertical gradients in CO and water vapor, decreasing with altitude and varying in time, but this water vapor does not originate as a product of the BB combustion itself. Due to a combination of conditions and mixing between the smoky, moist continental boundary layer and the dry and fairly clean upper-troposphere air above (~6 km), the smoky, humid air is transported by strong zonal winds and then advected over the SEA (to the ORACLES flight region) following largely isentropic trajectories. Hybrid Single-Particle Lagrangian Integrated Trajectory model (HYSPLIT) back trajectories support this interpretation. This work thus gives insights into the conditions and processes which cause water vapor to covary with plume strength. Better understanding of this relationship, including how it varies spatially and temporally, is important to accurately quantify direct, semi-direct, and indirect aerosol effects over this region.

54 ENVIRONMENTAL SCIENCES↗

Aerosol-Cloud Interactions From Aviation Soot Emissions

Current models estimate global aviation contributes approximately 5% to the total anthropogenic climate forcing, with aerosol-cloud interactions having the greatest effect. However, radiative forcing estimates from aviation aerosol-cloud interactions remain undetermined. There is an expected significant increase in aircraft emissions with aviation demand expected to rise by over 4% per year. Soot may play an important role in the ice nucleation of aircraft-induced cirrus formation due to a high emission rate, but the ice nucleating properties are poorly constrained. Understanding the microphysical processes leading to atmospheric ice crystal formation is crucial for the reliable parameterization of aerosol-cloud interactions in climate models due to their impact on precipitation and cloud radiative properties. Ice nucleation of aircraft-emitted soot is potentially affected by particle morphology with condensation of supercooled water occurring in pores followed by ice nucleation. However, soot has heterogeneous properties and undergoes atmospheric aging and oxidation that could change surface properties and contribute to complex ice nucleation processes. Further, this review synthesizes current knowledge of ice nucleation catalyzed by aviation in the cirrus regime and its effects on global radiative forcing. Further research is required to determine the ice nucleation and microphysical processes of cirrus cloud formation from aviation emissions in both controlled laboratory and field investigations to inform models for more accurate climate predictions and to provide efficient mitigation strategies.

54 ENVIRONMENTAL SCIENCES↗

Factors controlling marine aerosol size distributions and their climate effects over the northwest Atlantic Ocean region

Abstract. Aerosols over Earth's remote and spatially extensive ocean surfaces have important influences on planetary climate. However, these aerosols and their effects remain poorly understood, in part due to the remoteness and limited observations over these regions. In this study, we seek to understand factors that shape marine aerosol size distributions and composition in the northwest Atlantic Ocean region. We use the GEOS-Chem model with the TwO-Moment Aerosol Sectional (TOMAS) microphysics algorithm model to interpret measurements collected from ship and aircraft during the four seasonal campaigns of the North Atlantic Aerosols and Marine Ecosystems Study (NAAMES) conducted between 2015 and 2018. Observations from the NAAMES campaigns show enhancements in the campaign-median number of aerosols with diameters larger than 3 nm in the lower troposphere (below 6 km), most pronounced during the phytoplankton bloom maxima (May/June) below 2 km in the free troposphere. Our simulations, combined with NAAMES ship and aircraft measurements, suggest several key factors that contribute to aerosol number and size in the northwest Atlantic lower troposphere, with significant regional-mean (40–60∘ N and 20–50∘ W) cloud-albedo aerosol indirect effect (AIE) and direct radiative effect (DRE) processes during the phytoplankton bloom. These key factors and their associated simulated radiative effects in the region include the following: (1) particle formation near and above the marine boundary layer (MBL) top (AIE: −3.37 W m−2, DRE: −0.62 W m−2); (2) particle growth due to marine secondary organic aerosol (MSOA) as the nascent particles subside into the MBL, enabling them to become cloud-condensation-nuclei-sized particles (AIE: −2.27 W m−2, DRE: −0.10 W m−2); (3) particle formation and growth due to the products of dimethyl sulfide, above and within the MBL (−1.29 W m−2, DRE: −0.06 W m−2); (4) ship emissions (AIE: −0.62 W m−2, DRE: −0.05 W m−2); and (5) primary sea spray emissions (AIE: +0.04 W m−2, DRE: −0.79 W m−2). Our results suggest that a synergy of particle formation in the lower troposphere (particularly near and above the MBL top) and growth by MSOA contributes strongly to cloud-condensation-nuclei-sized particles with significant regional radiative effects in the northwest Atlantic. To gain confidence in radiative effect magnitudes, future work is needed to understand (1) the sources and temperature dependence of condensable marine vapors forming MSOA, (2) primary sea spray emissions, and (3) the species that can form new particles in the lower troposphere and grow these particles as they descend into the marine boundary layer.

54 ENVIRONMENTAL SCIENCES↗

Cloud Properties and Boundary Layer Stability Above Southern Ocean Sea Ice and Coastal Antarctica

Significant variability in climate predictions originates from the simulated cloud cover over the Southern Ocean. Historically, Southern Ocean cloud and aerosol properties have been less studied than their northern hemisphere counterparts, and cloud-sea-ice interactions over the Southern Ocean also remain largely unexamined. We used data from combined radar, lidar, radiometer, radiosonde, and ERA5 reanalysis profiles to investigate cloud property relationships to cloud temperature, sea-ice concentration, and boundary layer stability. Our findings show correlations between both cloud macrophysical properties and radiative effects and sea-ice concentration, and that the marine atmospheric boundary layer is more stable over higher sea-ice concentrations. Mixed-phase cloud frequency of occurrence was highest over the sea-ice zone at 15%, three times higher than over cold water south of the Antarctic Polar Front. For temperatures greater than –15°C, low-level, single-layer clouds were more likely to precipitate ice if they were coupled to cold-water or sea-ice surfaces than if they were decoupled from these surfaces, with the highest percentage of clouds precipitating ice observed over sea ice. These findings suggest a surface source of ice-nucleating particles at high southern latitudes that increases cloud glaciation probability. We discuss the implications of our results for future studies into the relationship between cloud properties, aerosols, sea ice, and boundary layer stability at high latitudes over the Southern Ocean.

54 ENVIRONMENTAL SCIENCES↗

The correlation between Arctic sea ice, cloud phase and radiation using A-Train satellites

Abstract. Climate warming has a stronger impact on Arctic climate and sea ice cover (SIC) decline than previously thought. Better understanding and characterization of the relationship between sea ice and clouds and the implications for surface radiation is key to improving our confidence in Arctic climate projections. Here we analyze the relationship between sea ice, cloud phase and surface radiation over the Arctic, defined as north of 60° N, using active- and passive-sensor satellite observations from three different datasets. We find that all datasets agree on the climatology of and seasonal variability in total and liquid-bearing (liquid and mixed-phase) cloud covers. Similarly, our results show a robust relationship between decreased SIC and increased liquid-bearing clouds in the lowest levels (below 3 km) for all seasons (strongest in winter) but summer, while increased SIC and ice clouds are positively correlated in two of the three datasets. A refined map correlation analysis indicates that the relationship between SIC and liquid-bearing clouds can change sign over the Bering, Barents and Laptev seas, likely because of intrusions of warm air from low latitudes during winter and spring. Finally, the increase in liquid clouds resulting from decreasing SIC is associated with enhanced radiative cooling at the surface. Our findings indicate that the newly formed liquid clouds reflect more shortwave (SW) radiation back to space compared to the surface, generating a cooling effect of the surface, while their downward longwave (LW) radiation is similar to the upward LW surface emission, which has a negligible radiative impact on the surface. This overall cooling effect should contribute to dampening future Arctic surface warming as SIC continues to decline.

54 ENVIRONMENTAL SCIENCES↗

Constraining the Twomey effect from satellite observations: issues and perspectives

Abstract. The Twomey effect describes the radiative forcing associated with a change in cloud albedo due to an increase in anthropogenic aerosol emissions. It is driven by the perturbation in cloud droplet number concentration (ΔNd, ant) in liquid-water clouds and is currently understood to exert a cooling effect on climate. The Twomey effect is the key driver in the effective radiative forcing due to aerosol–cloud interactions, but rapid adjustments also contribute. These adjustments are essentially the responses of cloud fraction and liquid water path to ΔNd, ant and thus scale approximately with it. While the fundamental physics of the influence of added aerosol particles on the droplet concentration (Nd) is well described by established theory at the particle scale (micrometres), how this relationship is expressed at the large-scale (hundreds of kilometres) perturbation, ΔNd, ant, remains uncertain. The discrepancy between process understanding at particle scale and insufficient quantification at the climate-relevant large scale is caused by co-variability of aerosol particles and updraught velocity and by droplet sink processes. These operate at scales on the order of tens of metres at which only localised observations are available and at which no approach yet exists to quantify the anthropogenic perturbation. Different atmospheric models suggest diverse magnitudes of the Twomey effect even when applying the same anthropogenic aerosol emission perturbation. Thus, observational data are needed to quantify and constrain the Twomey effect. At the global scale, this means satellite data. There are four key uncertainties in determining ΔNd, ant, namely the quantification of (i) the cloud-active aerosol – the cloud condensation nuclei (CCN) concentrations at or above cloud base, (ii) Nd, (iii) the statistical approach for inferring the sensitivity of Nd to aerosol particles from the satellite data and (iv) uncertainty in the anthropogenic perturbation to CCN concentrations, which is not easily accessible from observational data. This review discusses deficiencies of current approaches for the different aspects of the problem and proposes several ways forward: in terms of CCN, retrievals of optical quantities such as aerosol optical depth suffer from a lack of vertical resolution, size and hygroscopicity information, non-direct relation to the concentration of aerosols, difficulty to quantify it within or below clouds, and the problem of insufficient sensitivity at low concentrations, in addition to retrieval errors. A future path forward can include utilising co-located polarimeter and lidar instruments, ideally including high-spectral-resolution lidar capability at two wavelengths to maximise vertically resolved size distribution information content. In terms of Nd, a key problem is the lack of operational retrievals of this quantity and the inaccuracy of the retrieval especially in broken-cloud regimes. As for the Nd-to-CCN sensitivity, key issues are the updraught distributions and the role of Nd sink processes, for which empirical assessments for specific cloud regimes are currently the best solutions. These considerations point to the conclusion that past studies using existing approaches have likely underestimated the true sensitivity and, thus, the radiative forcing due to the Twomey effect.

54 ENVIRONMENTAL SCIENCES↗