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Marine cloud brightening (MCB) is the deliberate injection of aerosol particles into shallow marine clouds to increase their reflection of solar radiation and reduce the amount of energy absorbed by the climate system. From the physical science perspective, the consensus of a broad international group of scientists is that the viability of MCB will ultimately depend on whether observations and models can robustly assess the scale-up of local-to-global brightening in todays climate and identify strategies that will ensure an equitable geographical distribution of the benefits and risks associated with projected regional changes in temperature and precipitation. To address the physical science knowledge gaps required to assess the societal implications of MCB, we propose a substantial and targeted program of research-field and laboratory experiments, monitoring, and numerical modeling across a range of scales.

The climate effects of atmospheric aerosol particles serving as cloud condensation nuclei (CCN) depend on chemical composition and hygroscopicity, which are highly variable on spatial and temporal scales. Here we present global CCN measurements, covering diverse environments from pristine to highly polluted conditions. We show that the effective aerosol hygroscopicity, κ, can be derived accurately from the fine aerosol mass fractions of organic particulate matter (ϵorg) and inorganic ions (ϵinorg) through a linear combination, κ = ϵorg ⋅ κorg + ϵinorg ⋅ κinorg. In spite of the chemical complexity of organic matter, its hygroscopicity is well captured and represented by a global average value of κorg = 0.12 ± 0.02 with κinorg = 0.63 ± 0.01 as the corresponding value for inorganic ions. By showing that the sensitivity of global climate forcing to changes in κorg and κinorg is small, we constrain a critically important aspect of global climate modelling.

A technique is presented that uses attenuated backscatter profiles from the CALIOP satellite lidar to estimate cloud base heights of lower-troposphere liquid clouds (cloud base height below approximately 3 km). Even when clouds are thick enough to attenuate the lidar beam (optical thickness τ≥5), the technique provides cloud base heights by treating the cloud base height of nearby thinner clouds as representative of the surrounding cloud field. Using ground-based ceilometer data, uncertainty estimates for the cloud base height product at retrieval resolution are derived as a function of various properties of the CALIOP lidar profiles. Evaluation of the predicted cloud base heights and their predicted uncertainty using a second statistically independent ceilometer dataset shows that cloud base heights and uncertainties are biased by less than 10 %. Geographic distributions of cloud base height and its uncertainty are presented. In some regions, the uncertainty is found to be substantially smaller than the 480m uncertainty assumed in the A-Train surface downwelling longwave estimate, potentially permitting the most uncertain of the radiative fluxes in the climate system to be better constrained.

Over the past few decades, the geographical distribution of emissions of substances that alter the atmospheric energy balance has changed due to economic growth and air pollution regulations. Here, we show the resulting changes to aerosol and ozone abundances and their radiative forcing using recently updated emission data for the period 1990-2015, as simulated by seven global atmospheric composition models. The models broadly reproduce large-scale changes in surface aerosol and ozone based on observations (e.g.-1 to-3%yr-1 in aerosols over the USA and Europe). The global mean radiative forcing due to ozone and aerosol changes over the 1990-2015 period increased by +0.17±0.08Wm-2, with approximately one-third due to ozone. This increase is more strongly positive than that reported in IPCC AR5. The main reasons for the increased positive radiative forcing of aerosols over this period are the substantial reduction of global mean SO2 emissions, which is stronger in the new emission inventory compared to that used in the IPCC analysis, and higher black carbon emissions.

Cloud albedo susceptibility to droplet number perturbation remains a source of uncertainty in understanding aerosol–cloud interactions and thus both past and present climate states. Through the Energy Exascale Earth System Model (E3SM) v2 experiments, we probe the effects of competing processes on cloud albedo susceptibility of low-lying marine stratocumulus in the northeast Pacific. In present-day conditions, we find that increasing precipitation suppression by aerosols increases cloud albedo susceptibility, whereas increasing cloud sedimentation decreases it. By constructing a hypothetical model configuration exhibiting negative susceptibility under all conditions, we conclude that cloud albedo change due to aerosol perturbation cannot be predicted by present-day co-variabilities in E3SM v2. As such, our null result herein challenges the assumption that present-day climate observations are sufficient to constrain past states, at least in the context of cloud albedo changes to aerosol perturbation. [ABSTRACT FROM AUTHOR]

General circulation models' (GCMs) estimates of the liquid water path adjustment to anthropogenic aerosol emissions differ in sign from other lines of evidence. This reduces confidence in estimates of the effective radiative forcing of the climate by aerosol–cloud interactions (ERFaci). The discrepancy is thought to stem in part from GCMs' inability to represent the turbulence–microphysics interactions in cloud-top entrainment, a mechanism that leads to a reduction in liquid water in response to an anthropogenic increase in aerosols. In the real atmosphere, enhanced cloud-top entrainment is thought to be the dominant adjustment mechanism for liquid water path, weakening the overall ERFaci. We show that the latest generation of GCMs includes models that produce a negative correlation between the present-day cloud droplet number and liquid water path, a key piece of observational evidence supporting liquid water path reduction by anthropogenic aerosols and one that earlier-generation GCMs could not reproduce. However, even in GCMs with this negative correlation, the increase in anthropogenic aerosols from preindustrial to present-day values still leads to an increase in the simulated liquid water path due to the parameterized precipitation suppression mechanism. This adds to the evidence that correlations in the present-day climate are not necessarily causal. We investigate sources of confounding to explain the noncausal correlation between liquid water path and droplet number. These results are a reminder that assessments of climate parameters based on multiple lines of evidence must carefully consider the complementary strengths of different lines when the lines disagree. [ABSTRACT FROM AUTHOR]

Process-oriented observational constraints for the anthropogenic effective radiative forcing due to aerosol–cloud interactions (ERFaci) are highly desirable because the uncertainty associated with ERFaci poses a significant challenge to climate prediction. The contoured frequency by optical depth diagram (CFODD) analysis supports the evaluation of model representation of cloud liquid-to-rain conversion processes because the slope of a CFODD, generated from joint MODerate Resolution Imaging Spectroradiometer (MODIS)-CloudSat cloud retrievals, provides an estimate of cloud droplet collection efficiency in single-layer warm liquid clouds. Here, we present an updated CFODD analysis as an observational constraint on the ERFaci due to warm rain processes and apply it to the U.S. Department of Energy's Energy Exascale Earth System Model version 2 (E3SMv2). A series of sensitivity experiments shows that E3SMv2 droplet collection efficiencies and ERFaci are highly sensitive to autoconversion, i.e., the rate of mass transfer from cloud liquid to rain, yielding a strong correlation between the CFODD slope and the shortwave component of ERFaci (ERFaci SW ; Pearson's R=-0.91). E3SMv2's CFODD slope (0.20 ± 0.04) is in agreement with observations (0.20 ± 0.03). The strong sensitivity of ERFaci SW to the CFODD slope provides a useful constraint on highly uncertain warm rain processes, whereby ERFaci SW , constrained by MODIS-CloudSat, is estimated by calculating the intercept of the linear association between the ERFaci SW and the CFODD slopes, using the MODIS-CloudSat CFODD slope as a reference. [ABSTRACT FROM AUTHOR]

General circulation models (GCMs), unlike other lines of evidence, indicate that anthropogenic aerosols cause a global-mean increase in cloud liquid water path (퓛), and thus a negative adjustment to radiative forcing of the climate by aerosol–cloud interactions. In part 1 of this manuscript series, we showed that this is true even in models that reproduce the negative correlation observed in present-day internal variability of 퓛 and cloud droplet number concentration (Nd). We studied several possible confounding mechanisms that could explain the noncausal cloud–aerosol correlations in GCMs and that possibly contaminate observational estimates of radiative adjustments. Here, we perform single-column and full-atmosphere GCM experiments to investigate the causal model-physics mechanisms underlying the model radiative adjustment estimate. We find that both aerosol–cloud interaction mechanisms thought to be operating in real clouds – precipitation suppression and entrainment evaporation enhancement – are active in GCMs and behave qualitatively in agreement with physical process understanding. However, the modeled entrainment enhancement has a negligible global-mean effect. This raises the question whether the GCM estimate is incorrect due to parametric or base-state representation errors, or whether the process understanding gleaned from a limited set of canonical cloud cases is insufficiently representative of the diversity of clouds in the real climate. Regardless, even at limited resolution, the GCM physics appears able to parameterize the small-scale microphysics–turbulence interplay responsible for the entrainment enhancement mechanism. We suggest ways to resolve tension between current and future (storm-resolving) global modeling systems and other lines of evidence in synthesis climate projections. [ABSTRACT FROM AUTHOR]

Cloud albedo susceptibility to droplet number perturbation remains a source of uncertainty in understanding aerosol– cloud interactions, and thus climate states both past and present. Through E3SM v2 experiments, we probe the effects of competing parameterized processes on cloud albedo susceptibility of low-lying marine stratocumulus in the Northeast Pacific. In present-day conditions, we find that increasing precipitation suppression by aerosols increases cloud albedo susceptibility, whereas increasing cloud sedimentation decreases it. By constructing a hypothetical model configuration exhibiting negative susceptibility under all conditions, we conclude that cloud albedo change due to aerosol perturbation cannot be constrained by present-day co-variabilities in E3SM v2. As such, our null result herein challenges the assumption that present-day climate observations are sufficient to constrain past states, at least in the context of cloud albedo changes to aerosol perturbation. [ABSTRACT FROM AUTHOR]

Process-oriented observational constraints for the anthropogenic effective radiative forcing due to aerosol-cloud-interactions (ERFaci) are highly desirable because the large uncertainty associated with ERFaci poses a significant challenge to climate prediction. The satellite-based Contoured Frequency by Optical Depth Diagrams (CFODD) analysis was previously proposed to support evaluation of model representation of cloud liquid to rain conversion processes because the slope of a CFODD, generated from joint MODerate Resolution Imaging Spectroradiometer (MODIS)-CloudSat cloud retrievals, provides an estimate of cloud droplet collection efficiency in single-layer warm liquid clouds (SLWCs). Here we present an updated CFODD analysis as an observational constraint for the ERFaci due to warm rain processes and apply it to the U.S. Department of Energy's Energy Exascale Earth System Model version 2 (E3SMv2). Updates to the CFODD analysis include multiple changes to the SLWC detection algorithm for better consistency between MODIS-CloudSat observations and the satellite simulators, as well as the estimation of CFODD slopes using Random Sample Consensus robust linear regression. A series of sensitivity experiments shows that E3SMv2 droplet collection efficiencies and ERFaci are highly sensitive to the treatment of autoconversion, the rate of mass transfer from cloud liquid to rain, yielding a strong correlation between the CFODD slope and the shortwave component of ERFaci (Pearson's R = -0.91). We estimate the shortwave component of ERFaci (ERFaciSW), constrained by MODIS-CloudSat, by calculating the intercept of the linear association between E3SMv2 ERFaciSW and the CFODD slopes, using the MODIS-CloudSat CFODD slope as a reference. When E3SMv2's droplet collection efficiency is constrained to agree with the A-Train retrievals, ERFaciSW is reduced by 13 % in magnitude, indicating that correcting bias in the ERFaciSW due to autoconversion would bring E3SMv2's total ERFaci (-1.50 W m-2) into better agreement with the IPCC AR6 'very likely' range for ERFaci (-1.0 ± 0.7 W m-2). This study provides a new process-oriented observational constraint for ERFaci due to warm rain processes to reduce the uncertainty of climate predictions. [ABSTRACT FROM AUTHOR]

Uncertainties associated with the response of shallow clouds to global warming remain a great challenge for climate projection. Due to the small size of these clouds, parameterizations are required to represent them in both current‐ and next‐generation climate models. We present a quantitative evaluation of several important assumptions used in both mass‐flux and Assumed‐PDF Higher‐Order Closure parameterizations of shallow convection. We use large‐eddy simulations (LESs) of four different shallow convection regimes as benchmarks and apply a qt (total moisture)–w (vertical velocity) quadrant analysis technique to identify the "coherent structures" of moist and dry up/down‐drafts. The statistics of these coherent structures and the environment are then used to evaluate commonly used assumptions in mass‐flux parameterizations related to (a) the convective downdrafts and (b) the subplume variability of convective updrafts. For quantitative evaluation of the PDF closure used in AP‐HOCs, we perform offline calculations with the PDF closure used in the Cloud Layers Unified By Bi‐normals and the Simplified Higher‐Order Closure schemes by supplying the closure with statistical quantities directly calculated from the LESs. Then, the impact of parameterization assumptions embedded in the PDF closure in the same two categories is analyzed and understood through comparisons of the output from the closure with the statistics of the moist and dry up/down‐drafts from the LESs. Plain Language Summary: This study examines critically several key simplifying assumptions about convective downdrafts and small‐scale variability associated with shallow clouds that are made in two types of shallow convection parameterizations widely used in numerical weather and climate models and demonstrates quantitatively the impact of these assumptions on the parameterized cloud water content, depth, and turbulent transport. Key Points: A qt–w quadrant analysis is applied to identify convective coherent structures in large‐eddy simulations of various shallow cloud regimesStatistics from the quadrant analysis is used to evaluate assumptions in mass‐flux and Assumed‐PDF Higher‐Order Closure shallow convection parameterizationsSimplifying assumptions on convective downdrafts and subplume variability are linked to parameterization deficiencies [ABSTRACT FROM AUTHOR]

The impact of aerosol number concentration on cloud albedo is a persistent source of spread in global climate predictions due to multi-scale, interactive atmospheric processes that remain difficult to quantify. We use 5 years of geostationary satellite and surface retrievals at the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Eastern North Atlantic (ENA) site in the Azores to evaluate the representation of liquid cloud albedo susceptibility for overcast cloud scenes in DOE Energy Exascale Earth System Model version 1 (E3SMv1) and provide possible reasons for model-observation discrepancies. The overall distribution of surface 0.2 % CCN concentration values is reasonably simulated but simulated liquid water path (LWP) is lower than observed and layer-mean droplet concentration (Nd) comparisons are highly variable depending on the Nd retrieval technique. E3SMv1's cloud albedo is greater than observed for given LWP and Nd values due to a lesser cloud effective radius than observed. However, the simulated albedo response to Nd is suppressed due to a solar zenith angle (SZA)-Nd correlation created by the seasonal cycle that is not observed. Controlling for this effect by examining the cloud optical depth (COD) shows that E3SMv1's COD response to CCN concentration is greater than observed. For surface-based retrievals, this is only true after controlling for cloud adiabaticity because E3SMv1's adiabaticities are much lower than observed. Assuming a constant adiabaticity in surface retrievals as done in TOA retrievals narrows the retrieved lnNd distribution, which increases the cloud albedo sensitivity to lnNd to match the TOA sensitivity. The greater sensitivity of COD to CCN is caused by a greater Twomey effect in which the sensitivity of Nd to CCN is greater than observed for TOA-retrieved Nd, and once model-observation adiabaticity differences are removed, this is also true for surface-retrieved Nd. The LWP response to Nd in E3SMv1 is overall negative as observed. Despite reproducing the observed LWP-Nd relationship, observed clouds become much more adiabatic as Nd increases while E3SMv1 clouds do not, associated with more heavily precipitating clouds that are partially but not completely caused by deeper clouds and weaker inversions in E3SMv1. These cloud property differences indicate that the negative LWP-Nd relationship is likely not caused by the same mechanisms in E3SMv1 and observations. The negative simulated LWP response also fails to mute the excessively strong Twomey effect, highlighting potentially important confounding factor effects that likely render the LWP-Nd relationship non-causal. Nd retrieval scales and assumptions, particularly related to cloud adiabaticity, contribute to substantial spreads in the model-observation comparisons, though enough consistency exists to suggest that aerosol activation and convective drizzle processes are critical areas to focus E3SMv1 development for improving the fidelity of aerosol-cloud interactions in E3SM. [ABSTRACT FROM AUTHOR]

Over the remote Southern Ocean, cloud feedbacks contribute substantially to Earth system model (ESM) radiative biases. The evolution of low Southern Ocean clouds (cloud top heights < ~ 3 km) is strongly modulated by precipitation and/or evaporation, which act as the primary sink of cloud condensate. Constraining precipitation processes in ESMs requires robust observations suitable for process-level evaluations. A year-long subset (April 2016 – March 2017) of ground-based profiling instrumentation deployed during the Macquarie Island Cloud and Radiation Experiment (MICRE) field campaign (54.5° S, 158.9° E) combines a 95 GHz (W-band) Doppler cloud radar, two lidar ceilometers, and balloon-borne soundings to quantify the occurrence frequency of precipitation from liquid-phase cloud base. Liquid-based clouds at Macquarie Island precipitate ~ 70 % of the time, with deeper and colder clouds precipitating more frequently and at a higher intensity compared to thinner and warmer clouds. Supercooled cloud layers precipitate more readily than layers with cloud top temperatures > 0 °C, regardless of the geometric thickness of the layer, and also evaporate more frequently. We further demonstrate an approach to employ these observational constraints for evaluation of a 9-year GISS-ModelE3 ESM simulation. Model output is processed through the Earth Model Column Collaboratory (EMC2) radar and lidar instrument simulator with the same instrument specifications as those deployed during MICRE, therefore accounting for instrument sensitivities and ensuring a coherent comparison. Relative to MICRE observations, the ESM produces a smaller cloud occurrence frequency, smaller precipitation occurrence frequency, and greater sub-cloud evaporation. The lower precipitation occurrence frequency by the ESM relative to MICRE contrasts with numerous studies that suggest a ubiquitous bias by ESMs to precipitate too frequently over the SO when compared with satellite-based observations, likely owing to sensitivity limitations of space-borne instrumentation and different sampling methodologies for ground- versus space-based observations. Despite these deficiencies, the ESM reproduces the observed tendency for deeper and colder clouds to precipitate more frequently and at a higher intensity. The ESM also reproduces specific cloud regimes, including near-surface clouds that account for ~ 25 % of liquid-based clouds during MICRE and optically thin, non-precipitating clouds that account for ~ 27 % of clouds with bases higher than 250 m. We suggest that the demonstrated framework, which merges observations with appropriately constrained model output, is a valuable approach to evaluate processes responsible for cloud radiative feedbacks in ESMs. [ABSTRACT FROM AUTHOR]

Over the remote Southern Ocean, cloud feedbacks contribute substantially to Earth system model (ESM) radiative biases. The evolution of low Southern Ocean clouds (cloud top heights < ~ 3 km) is strongly modulated by precipitation and/or evaporation, which act as the primary sink of cloud condensate. Constraining precipitation processes in ESMs requires robust observations suitable for process-level evaluations. A year-long subset (April 2016 - March 2017) of ground-based profiling instrumentation deployed during the Macquarie Island Cloud and Radiation Experiment (MICRE) field campaign (54.5° S, 158.9° E) combines a 95 GHz (W-band) Doppler cloud radar, two lidar ceilometers, and balloon-borne soundings to quantify the occurrence frequency of precipitation from liquid-phase cloud base. Liquid-based clouds at Macquarie Island precipitate ~ 70 % of the time, with deeper and colder clouds precipitating more frequently and at a higher intensity compared to thinner and warmer clouds. Supercooled cloud layers precipitate more readily than layers with cloud top temperatures > 0 °C, regardless of the geometric thickness of the layer, and also evaporate more frequently. We further demonstrate an approach to employ these observational constraints for evaluation of a 9-year GISS-ModelE3 ESM simulation. Model output is processed through the Earth Model Column Collaboratory (EMC²) radar and lidar instrument simulator with the same instrument specifications as those deployed during MICRE, therefore accounting for instrument sensitivities and ensuring a coherent comparison. Relative to MICRE observations, the ESM produces a smaller cloud occurrence frequency, smaller precipitation occurrence frequency, and greater sub-cloud evaporation. The lower precipitation occurrence frequency by the ESM relative to MICRE contrasts with numerous studies that suggest a ubiquitous bias by ESMs to precipitate too frequently over the SO when compared with satellite-based observations, likely owing to sensitivity limitations of space-borne instrumentation and different sampling methodologies for ground- versus space-based observations. Despite these deficiencies, the ESM reproduces the observed tendency for deeper and colder clouds to precipitate more frequently and at a higher intensity. The ESM also reproduces specific cloud regimes, including near-surface clouds that account for ~ 25 % of liquid-based clouds during MICRE and optically thin, non-precipitating clouds that account for ~ 27 % of clouds with bases higher than 250 m. We suggest that the demonstrated framework, which merges observations with appropriately constrained model output, is a valuable approach to evaluate processes responsible for cloud radiative feedbacks in ESMs. [ABSTRACT FROM AUTHOR]

A Lagrangian framework is used to evaluate aerosol-cloud interactions in the U.S. Department of Energy's Energy Exascale Earth System Model (E3SM) version 1 (E3SMv1) for measurements taken at Graciosa Island in the Azores where a U.S. Department of Energy Atmosphere Radiation Measurement (ARM) site is located. This framework uses direct measurements of CCN (instead of relying on satellite retrievals of aerosol optical depth) and incorporates a suite of ground-based ARM measurements, satellite retrievals, and meteorological reanalysis products that when applied to over a 1,500 trajectories provides key insights into the evolution of low-level clouds and aerosol radiative forcing that is not feasible from a traditional Eulerian analysis framework. Significantly lower concentrations (40 %) of surface cloud condensation nuclei (CCN) are measured when precipitation rates in 48-hour back trajectories average above 1.2 mm/d in the Integrated Multi-satellitE Retrievalsfor GPM (IMERG) product. The depletion of CCN when precipitation rates are elevated is nearly twice as large in the ARM observations compared to E3SMv1 simulations. The model CCN bias remains significant despite modifying the autoconversion and accretion rates in warm clouds. As the clouds in trajectories associated with larger surface-based CCN advect away from Graciosa Island they maintain higher values of droplet number concentrations (Nd) over multiple days in observations and E3SM simulations compared to trajectories that start with lower CCN concentrations. The response remains robust even after controlling for meteorological factors such as lower troposphere stability, the degree of cloud coupling with the surface, and island wake effects. E3SMv1 simulates a multi-day aerosol effect on clouds and a Twomey radiative effect that is within 30 % of the ARM and satellite observations. However, the mean cloud droplet concentration is more than 2–3 times larger than in the observations. While Twomey radiative effects are similar amongst autoconversion and accretion sensitivity experiments the liquid water path and cloud fraction adjustments are positive when using a regression model as opposed to negative when using the present-day minus pre-industrial day aerosol emissions approach. This result suggests that tuning the autoconversion and accretion alone are unlikely to produce the desired aerosol susceptibilities in E3SMv1. [ABSTRACT FROM AUTHOR]