The accurate representation of cloud droplet number concentration (Nd) is crucial for predicting future climate. However, models often underestimate Nd over the Southern Ocean (SO), where natural sources dominate, and aerosols are composed primarily of marine biogenic sulfate and sea spray. This study uses a range of diverse datasets to evaluate and untangle biases in E3SMv2 simulated clouds, aerosols, and sulfur species. The default E3SMv2 underestimates Nd over SO by a factor of 2 when compared with observations in 3km-resolution simulations. Updating the dimethyl sulfide (DMS) emission and chemistry leads to a better agreement between the model and the observations in Nd and boundary layer aerosols, but low biases persist in the free tropospheric aerosol concentrations larger than 70 nm, possibly attributable to insufficient particle growth. Preliminary evaluation also reveals biases in simulated sulfur species, including overestimation in DMS at high latitudes, and in simulated sulfate mass concentration, highlighting the necessity for further efforts to improve the model treatment of relevant processes.

A document by Isabel L. McCoy. Click on the document to view its contents.

Cloud responses to surface-based sources of aerosol perturbation depend in part on the characteristics of the aerosol transport to cloud base and the resulting spatial and temporal distribution of aerosol. However, interactions among aerosol, cloud, and turbulence processes complicate the prediction of this aerosol transport and can obscure diagnosis of the aerosols' effects on cloud and turbulence properties. Here, scenarios of plume injection below a marine stratocumulus cloud are modeled using large eddy simulations coupled to a prognostic bulk aerosol and cloud microphysics scheme. Both passive plumes, consisting of an inert tracer, and active plumes are investigated, where the latter are representative of saltwater droplet plumes such as have been proposed for marine cloud brightening. Passive plume scenarios show a spurious in-plume cloud brightening due solely to the connections between updrafts, cloud condensation, and scalar transport. Numerical sensitivities are first assessed to establish a suitable model configuration. Then sensitivity to particle injection rate is investigated. Trade-offs are identified between the number of injected particles and the suppressive effect of droplet evaporation on plume loft and spread. Furthermore, as the in-plume brightening effect does not depend significantly on injection rate given a suitable definition of perturbed versus unperturbed regions of the flow, plume area is a key controlling factor on the overall cloud brightening effect of an aerosol perturbation.

Precipitation plays an important role in various processes over the Southern Ocean (SO), ranging from the hydrological cycle to cloud and aerosol processes. The main objective of this study is to characterize SO precipitation properties. We use data from the Southern Ocean Clouds Radiation Aerosol Transport Experimental Study (SOCRATES), and leverage observations from airborne radar, lidar, and in situ probes. For the cold-topped clouds (cloud-top-temperature < 0°C), the phase of precipitation with reflectivity > 0 dBZ is predominately ice, while reflectivity < -10 dBZ is predominately liquid. Liquid-phase precipitation properties are retrieved where radar and lidar are zenith-pointing. The power-law relationships between reflectivity (Z) and rain rate (R) are developed, and the derived Z-R relationships show vertical dependence and sensitivity to the intermediate drops (diameters between 10-40 μm). Using derived Z-R relationships, reflectivity-velocity (ZV) retrieval method, and a radar-lidar retrieval method, we derive rain rate and other precipitation properties. The retrieved rain rate from all three methods shows good agreement with in-situ aircraft estimates. Rain rate features the prevalence of light precipitation (<0.1 mm hr-1). We examine the vertical distribution of precipitation properties, and found that rain rate, precipitation number concentration, precipitation liquid water all decreases as one gets closer to the surface, while precipitation size and width increases. We also examine how cloud base rain rate (RCB) depends on cloud depth (H) and aerosol concentration (Na) for particles with diameter greater than 70nm, and we find a linear relationship between RCB and H3.6Na-1.

Aerosol increases over the 20th century delayed the rate at which Earth warmed as a result of increases in greenhouse gases (GHGs). Aggressive aerosol mitigation policies arrested aerosol radiative forcing from ~1980 to ~2010. Recent evidence supports decreases in forcing magnitude since then. Using the approximate partial radiative perturbation (APRP) method, future shortwave aerosol effective radiative forcing changes are isolated from other shortwave changes in an 18-member ensemble of ScenarioMIP projections from phase 6 of the Coupled Model Intercomparison Project (CMIP6). APRP-derived near-term (2020-2050) aerosol forcing trends are correlated with published model emulation values but are 30-50% weaker. Differences are likely explained by location shifts of aerosol-impacting emissions and their resultant influences on susceptible clouds. Despite weaker changes, implementation of aggressive aerosol cleanup policies will have a major impact on global warming rates over 2020-2050. APRP-derived aerosol radiative forcings are used together with a forcing and impulse response model to estimate global temperature trends. Strong mitigation of GHGs, as in SSP1-2.6, likely prevents warming exceeding 2C since preindustrial but the strong aerosol cleanup in this scenario increases the probability of exceeding 2C by 2050 from near zero without aerosol changes to 6% with cleanup. When the same aerosol forcing is applied to a more likely GHG forcing scenario (i.e., SSP2-4.5), aggressive aerosol cleanup more than doubles the probability of reaching 2C by 2050 from 30% to 80%. It is thus critical to quantify and simulate the impacts of changes in aerosol radiative forcing over the next few decades.

Low marine clouds are a major source of uncertainty in cloud feedbacks across climate models and in forcing by aerosol-cloud interactions. The evolution of these clouds and their response to aerosol are sensitive to the ambient environmental conditions, so it is important to be able to determine different responses over a representative set of conditions. Here, we propose a novel approach to encompassing the broad range of conditions present in low marine cloud regions, by building a library of observed environmental conditions. This approach can be used, for example, to more systematically test the fidelity of Large Eddy Simulations (LES) in representing these clouds. ERA5 reanalysis and various satellite observations are used to extract and derive macrophysical and microphysical cloud-controlling variables (CCVs) such as SST, estimated inversion strength (EIS), subsidence, and cloud droplet number concentrations. A few locations in the stratocumulus (Sc) deck region of the Northeast Pacific during summer are selected to fill out a phase space of CCVs. Thereafter, Principal Component Analysis (PCA) is applied to reduce the dimensionality and to select a reduced set of components that explain most of the variability among CCVs in order to efficiently select cases for LES simulations that encompass the observed CCV phase space. From this phase space, 75-100 cases with distinct environmental conditions will be selected and used to initialize 2-day LES modeling to provide a spectrum of aerosol-cloud interactions and Sc-to-Cumulus transition under observed ambient conditions. Such a large number of simulations will help create statistics to assess how well the LES can simulate the cloud lifecycle when constrained by the ‘best estimate’ of the environmental conditions, and how sensitive the modeled clouds are to changes in these driving fields.

Observed stratocumulus to cumulus transitions (SCT) and their sensitivity to aerosols are studied using a Large-Eddy Simulation (LES) model that simulates the aerosol lifecycle, including aerosol sources and sinks. To initialize, force, and evaluate the LES, we used a combination of reanalysis, satellite, and aircraft data from the 2015 Cloud System Evolution in the Trades field campaign over the Northeast Pacific. The simulations follow two Lagrangian trajectories from initially overcast stratocumulus to the tropical shallow cumulus region near Hawaii. The first trajectory is characterized by an initially clean, well-mixed stratocumulus-topped marine boundary layer (MBL), then continuous MBL deepening and precipitation onset followed by a clear SCT and a consistent reduction of aerosols that ultimately leads to an ultra-clean layer in the upper MBL. The second trajectory is characterized by an initially polluted and decoupled MBL, weak precipitation, and a late SCT. Overall, the LES simulates the observed general MBL features. Sensitivity studies with different aerosol initial and boundary conditions reveal aerosol-induced changes in the transition, and albedo changes are decomposed into the Twomey effect and adjustments of cloud liquid water path and cloud fraction. Impacts on precipitation play a key role in the sensitivity to aerosols: for the first case, runs with enhanced aerosols exhibit distinct changes in microphysics and macrophysics such as enhanced cloud droplet number concentration, reduced precipitation, and delayed SCT. Cloud adjustments are dominant in this case. For the second case, enhancing aerosols does not affect cloud macrophysical properties significantly, and the Twomey effect dominates.

Future precipitation changes are controlled by the atmospheric energy budget, with temperature, water vapor, and absorbing aerosols playing dominant roles in driving radiative changes. Atmospheric energy budgets are calculated for different Shared Socioeconomic Pathways (SSPs) using ScenarioMIP projections from phase 6 of the Climate Model Intercomparison Project and are used to quantify the influence of 21st century aerosol cleanup on precipitation. Absorbing aerosol influences on shortwave absorption are isolated from the effects of water vapor. Apparent hydrologic sensitivity is ~40% higher for the “Middle of the Road” (SSP2-4.5) scenario with aerosol cleanup than for the “Regional Rivalry” (SSP3-7.0) scenario that maintains aerosol. Regionally, cleanup-induced changes in the atmospheric energy budget are of a similar magnitude to the precipitation increases themselves and are larger than the influence of changes in atmospheric circulation. Policy choices about future absorbing aerosol emissions will therefore have major impacts on global and regional precipitation changes.

Controls on pristine aerosol over the Southern Ocean (SO) are critical for constraining the strength of global aerosol indirect forcing. Observations of summertime SO clouds and aerosols in synoptically varied conditions during the 2018 SOCRATES aircraft campaign reveal novel mechanisms influencing pristine aerosol-cloud interactions. The SO free troposphere (3-6 km) is characterized by widespread, frequent new particle formation events contributing to much larger concentrations (≥ 1000 mg-1) of condensation nuclei (diameters > 0.01 μm) than in typical sub-tropical regions. Synoptic-scale uplift in warm conveyor belts and sub-polar vortices lifts marine biogenic sulfur-containing gases to free-tropospheric environments favorable for generating Aitken-mode aerosol particles (0.01-0.1 μm). Free-tropospheric Aitken particles subside into the boundary layer, where they grow in size to dominate the sulfur-based cloud condensation nuclei (CCN) driving SO cloud droplet number concentrations (Nd ~ 60-100 cm-3). Evidence is presented for a hypothesized Aitken-buffering mechanism which maintains persistently high summertime SO Nd against precipitation removal through CCN replenishment from activation and growth of boundary layer Aitken particles. Nudged hindcasts from the Community Atmosphere Model (CAM6) are found to underpredict Aitken and accumulation mode aerosols and Nd, impacting summertime cloud brightness and aerosol-cloud interactions and indicating incomplete representations of aerosol mechanisms associated with ocean biology.

Following the emergence of a novel coronavirus in Wuhan, the People’s Republic of China instituted a number of strict lockdown and more general socio-economic shutdown measures throughout the country starting in late January and continuing into February 2020 in order to arrest the spread of the disease. This resulted in a sharp economic contraction unparalleled in recent Chinese history. Satellite remote sensing shows that nitrogen oxide pollution declined by an unprecedented amount (~50% regionally) from its expected unperturbed value, but regional-scale column aerosol loadings and cloud microphysical properties were not detectably affected. The disparate impact may be tied to differential economic impacts of the shutdown, in which the transportation sector, a disproportionate source of nitrogen oxide emissions, underwent drastic declines (~90% reductions in passenger traffic), whereas industry and power generation, responsible for >90% of particulate emissions, were relatively less affected (~10% reductions in electricity and thermal power generation).

A new Aitken mode aerosol scheme is developed for a large eddy simulation (LES) model in order to better investigate cloud-aerosol interactions in the marine boundary layer and to study the Aitken buffering hypothesis of McCoy et al. (2021). This scheme extends the single-mode two-moment prognostic aerosol scheme of Berner et al. (2013). Nine prognostic variables represent accumulation and Aitken log-normal aerosol modes in air and droplets as well as 3 gas species. Scavenging of interstitial aerosol by cloud and rain drops and coagulation of dry aerosol are treated using the scheme described in B13. The scheme includes a simple chemistry model with gas phase H2SO4, SO2, and DMS as prognostic variables to capture basic influences of sulfur chemistry on the model aerosols. Primary nucleation of H2SO4 aerosol particles from gas-phase H2SO4 is neglected. A deep, precipitating stratocumulus case (VOCALS RF06) is used to test the new scheme. The presence of the Aitken mode aerosol increases the cloud droplet concentration through activation of the larger Aitken particles and delays the creation of an ultraclean, strongly precipitating cumulus state. Scavenging of dry accumulation and Aitken particles by cloud and precipitation droplets accelerates the collapse. Increasing either the above-inversion Aitken concentration or the surface Aitken flux increases the Aitken population in the boundary layer and prevents the transition to an ultraclean state.

A supervised neural network algorithm is used to categorize near-global satellite retrievals into three mesoscale cellular convective (MCC) cloud morphology patterns. At constant cloud amount, morphology patterns differ in brightness associated with the amount of optically-thin cloud features. Environmentally-driven transitions from closed MCC to other morphology patterns, typically accompanied by more optically-thin cloud features, are used as a framework to quantify the morphology contribution to the optical depth component of the shortwave cloud feedback. A marine heat wave is used as an out-of-sample test of closed MCC occurrence predictions. Morphology shifts in optical depth between 65°S - 65°N under projected environmental changes (i.e., from an abrupt quadrupling of CO2) assuming constant cloud cover contributes between 0.04-0.07 W/m2/K (aggregate of 0.06) to the global mean cloud feedback.