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Aerosol and Cloud Interaction Observed From High Spectral Resolution Lidar Data

Recent studies utilizing satellite retrievals have shown a strong correlation between aerosol optical depth (AOD) and cloud cover. However, these retrievals from passive sensors are subject to many limitations, including cloud adjacency (or 3D) effects, possible cloud contamination, uncertainty in the AOD retrieval. Some of these limitations do not exist in High Spectral Resolution Lidar (HSRL) observations; for instance, HSRL observations are not a ected by cloud adjacency effects, are less prone to cloud contamination, and offer accurate aerosol property measurements (backscatter coefficient, extinction coefficient, lidar ratio, backscatter Angstrom exponent,and aerosol optical depth) at a neospatial resolution (less than 100 m) in the vicinity of clouds. Hence, the HSRL provides an important dataset for studying aerosol and cloud interaction. In this study, we statistically analyze aircraft-based HSRL profiles according to their distance from the nearest cloud, assuring that all profile comparisons are subject to the same large-scale meteorological conditions. Our results indicate that AODs from HSRL are about 17% higher in the proximity of clouds (approximately 100 m) than far away from clouds (4.5 km), which is much smaller than the reported cloud 3D effect on AOD retrievals. The backscatter and extinction coefficients also systematically increase in the vicinity of clouds, which can be explained by aerosol swelling in the high relative humidity (RH) environment and/or aerosol growth through in cloud processing (albeit not conclusively). On the other hand, we do not observe a systematic trend in lidar ratio; we hypothesize that this is caused by the opposite effects of aerosol swelling and aerosol in-cloud processing on the lidar ratio. Finally, the observed backscatter Angstrom exponent (BAE) does not show a consistent trend because of the complicated relationship between BAE and RH. We demonstrate that BAE should not be used as a surrogate for Angstrom exponent, especially at high RH.

Su, Wenying↗

Significance of aerosol radiative effect in energy balance control on global precipitation change

Historical changes of global precipitation in the 20th century simulated by a climate model are investigated. The results simulated with alternate configurations of cloud microphysics are analyzed in the context of energy balance controls on global precipitation, where the latent heat changes associated with the precipitation change is nearly balanced with changes to atmospheric radiative cooling. The atmospheric radiative cooling is dominated by its clear-sky component, which is found to correlate with changes to both column water vapor and aerosol optical depth (AOD). The water vapor-dependent component of the clear-sky radiative cooling is then found to scale with global temperature change through the Clausius–Clapeyron relationship. This component results in a tendency of global precipitation increase with increasing temperature at a rate of approximately 2%K -1 . Another component of the clear-sky radiative cooling, which is well correlated with changes to AOD, is also found to vary in magnitude among different scenarios with alternate configurations of cloud microphysics that controls the precipitation efficiency, a major factor influencing the aerosol scavenging process that can lead to different aerosol loadings. These results propose how different characteristics of cloud microphysics can cause different aerosol loadings that in turn perturb global energy balance to significantly change global precipitation. This implies a possible coupling of aerosol–cloud interaction with aerosol–radiation interaction in the context of global energy balance.

54 ENVIRONMENTAL SCIENCES↗

Cloud Regimes as a Tool for Systematic Study of Various Aerosol-Cloud-Precipitation Interactions

Systematic changes of clouds and precipitation are notoriously difficult to ascribe to aerosols. This presentation will showcase yet one more attempt to at least credibly detect the signal of aerosol-cloud-precipitation interactions. We surmise that the concept of cloud regimes (CRs) is appropriate to conduct such an investigation. Previous studies focused on what we call here dynamical CRs, and while we continue to adopt those too for our analysis, we have found that a different way of organizing cloud systems, namely via microphysical regimes is also promising. Our analysis relies on MODIS Collection 6 Level-3 data for clouds and aerosols, and TRMM-TMPA data for precipitation. The regimes are derived by applying clustering analysis on MODIS joint histograms, and once each grid cell is assigned a regime, aerosol and precipitation data can be spatiotemporally matched and composited by regime. The composites of various cloud and precipitation variables for high (upper quartile of distribution) and low (lower quartile) aerosol loadings can then be contrasted. We seek evidence of aerosol effects both in regimes with large fractions of deep ice-rich clouds, as well as regimes where low liquid phase clouds dominate. Signals can be seen, especially when the analysis is broken by land-ocean and when additional filters are applied, but there are of course caveats which will be discussed.

cloud regimes↗

Chemical Imaging of Atmospheric Organic Particles in the Eastern North Atlantic Field Campaign Report

The ability to reliably predict future climate is hindered, in major part, by an insufficient understanding of atmospheric aerosol-radiation interactions and aerosol-cloud interactions. (IPCC 2013; Bony and Dufresne 2005) Factors affecting marine stratocumulus clouds are particularly important given that they are the dominant cloud type globally. Global climate models frequently misrepresent ubiquitous marine stratocumulus clouds for a variety of reasons, including a lack of understanding of how these cloud properties change with aerosol cloud condensation nuclei (CCN) concentration and composition.(Nam et al. 2012) Limited information is available regarding the sources of CCN in remote regions where marine stratocumulus clouds dominate. Measurements in these marine locations, which are periodically influenced by anthropogenic emissions, provide additional opportunity to study the impact of humans on cloud characteristics. The U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility Eastern North Atlantic (ENA) observatory on Graciosa Island in the Azores is well suited to study these problems. The ENA site is exposed to a multitude of air masses as well as a variety of cloud regimes, as documented by passive and active satellite cloud retrieval. (Tselioudis et al. 2013) Thus, placing detailed aerosol and cloud measurements at the ARM ENA site may help gain a better understanding of the CCN budget and cloud interactions in remote environments. To provide detailed information on aerosol morphology, composition, and microphysical properties, size- segregated sampling was carried out at the ENA observatory on Graciosa Island during two intensive operating periods (IOPs). IOP1 occurred from June 17 to July 18, 2017, and IOP2 occurred from January 9 to February 21, 2018. Daytime and nighttime sampling were carried out separately to investigate any diurnal differences of aerosol composition due to differing meteorology. For both IOPs, a micro-orifice uniform deposit impactor (MOUDI) was used to collect particles for microscopic and microphysical analysis. A variety of microscopic substrates (formvar coated copper grids, silicon chips, silicon nitride windows, or molybdenum substrates) were used. Microscopic chemical characterization was carried out using computer-controlled scanning electron microscopy coupled with energy-dispersive X-ray spectroscopy (CCSEM-EDX) and the synchrotron-based scanning transmission X-ray microscopy coupled with near-edge X-ray absorption spectroscopy (STXM-NEXAFS). (Laskin et al. 2006; Kilcoyne et al. 2003; Moffet et al. 2010) Two light sources were used for this analysis: 1) the Advanced Light Source at Lawrence Berkeley National Laboratory, and 2) The Canadian Light Source.

Eastern North Atlantic, ACE-ENA field campaign, Gr↗

Observations of Aerosol-Radiation-Cloud Interactions in the South-East Atlantic: First Results from the ORACLES Deployments in 2016 and 2017

Southern Africa produces almost a third of the Earths biomass burning (BB) aerosol particles. Particles lofted into the mid-troposphere are transported westward over the South-East (SE) Atlantic, home to one of the three permanent subtropical stratocumulus (Sc) cloud decks in the world. The SE Atlantic stratocumulus deck interacts with the dense layers of BB aerosols that initially overlay the cloud deck, but later subside and often mix into the clouds. These interactions include adjustments to aerosol-induced solar heating and microphysical effects, and their global representation in climate models remains one of the largest uncertainties in estimates of future climate. Hence, new observations over the SE Atlantic have significant implications for regional and global climate change predictions.The low-level clouds in the SE Atlantic have limited vertical extent and therefore present favorable conditions for their exploration with remote sensing. On the other hand, the normal coexistence of BB aerosols and Sc clouds in the same scene also presents significant challenges to conventional remote sensing techniques. We describe first results from NASAs airborne ORACLES (ObseRvations of Aerosols Above Clouds and Their IntEractionS) deployments in September 2016 and August 2017. We emphasize the unique role of polarimetric observations by two instruments, the Research Scanning Polarimeter (RSP) and the Airborne Multi-angle SpectroPolarimeter Imager (AirMSPI), and describe how these instruments help address specific ORACLES science objectives. Initial assessments of polarimetric observation accuracy for key cloud and aerosol properties will be presented, in as far as the preliminary nature of measurements permits.

Redemann, Jens↗

TAMU TRACER: Targeted Mobile Measurements to Isolate the Impacts of Aerosols and Meteorology on Deep Convection

Difficulty in using observations to isolate the impacts of aerosols from meteorology on deep convection often stems from inability to resolve the spatiotemporal variations in the environment serving as the storm’s inflow region. During the DOE TRacking Aerosol Convection interactions ExpeRiment (TRACER) in June-September 2022, a Texas A&M University (TAMU) team conducted a mobile field campaign to characterize the meteorological and aerosol variability in airmasses that serve as inflow to convection across the ubiquitous mesoscale boundaries associated with the sea- and bay-breezes in the Houston, Texas, region. These boundaries propagate inland over the fixed DOE Atmospheric Radiation Measurement (ARM) sites. However, convection occurs on either or both the continental or maritime sides or along the boundary. The maritime and continental airmasses serving as convection inflow may be quite distinct, with different meteorological and aerosol characteristics that fixed-site measurements cannot simultaneously sample. Thus, a primary objective of TAMU TRACER was to provide mobile measurements similar to those at the fixed sites, but in the opposite airmass across these moving mesoscale boundaries. TAMU TRACER collected radiosonde, lidar, aerosol, cloud condensation nuclei (CCN), and ice nucleating particle (INP) measurements on 29 enhanced operations days covering a variety of maritime, continental, outflow, and pre-frontal airmasses. This paper summarizes the TAMU TRACER deployment and measurement strategy, instruments, available datasets, and provides sample cases highlighting differences between these mobile measurements and those made at the ARM sites. We also highlight the exceptional TAMU TRACER undergraduate student participation in high impact learning activities through forecasting and field deployment opportunities.

54 ENVIRONMENTAL SCIENCES↗

Aerosol-Radiation-Cloud Interactions in the South-East Atlantic: Results from the ORACLES-2016 Deployment and a First Look at ORACLES-2017 and Beyond

Seasonal biomass burning (BB) in Southern Africa during the Southern hemisphere spring produces almost a third of the Earth's BB aerosol particles. These particles are lofted into the mid-troposphere and transported westward over the South-East (SE) Atlantic, where they interact with one of the three semi-permanent subtropical stratocumulus (Sc) cloud decks in the world. These interactions include adjustments to aerosol-induced solar heating and microphysical effects. The representation of these interactions in climate models remains highly uncertain, because of the scarcity of observational constraints on both, the aerosol and cloud properties, and the governing physical processes. The first deployment of the NASA P-3 and ER-2 aircraft in the ORACLES (ObseRvations of Aerosols Above Clouds and Their IntEractionS) project in August/September of 2016 has started to fill this observational gap by providing an unprecedented look at the SE Atlantic cloud-aerosol system. We provide an overview of the first deployment, highlighting aerosol absorptive and cloud-nucleating properties, their vertical distribution relative to clouds, the locations and degree of aerosol mixing into clouds, cloud changes in response to such mixing, and cloud top stability relationships to the aerosol. We also expect to describe preliminary results of the second ORACLES deployment from Sao Tome and Pri­ncipe in August 2017. We will make an initial assessment of the differences and similarities of the BB plume and cloud properties as observed from a deployment site near the plume's northern edge. We will conclude with an outlook for the third ORACLES deployment in October 2018.

Redemann, Jens↗

Tethered balloon measurements reveal enhanced aerosol occurrence aloft interacting with Arctic low-level clouds

Low-level clouds in the Arctic affect the surface energy budget and vertical transport of heat and moisture. The limited availability of cloud-droplet-forming aerosol particles strongly impacts cloud properties and lifetime. Vertical particle distributions are required to study aerosol–cloud interaction over sea ice comprehensively. This article presents vertically resolved measurements of aerosol particle number concentrations and sizes using tethered balloons. The data were collected during the Multidisciplinary drifting Observatory for the Study of Arctic Climate expedition in the summer of 2020. Thirty-four profiles of aerosol particle number concentration were observed in 2 particle size ranges: 12–150 nm (N 12−150 ) and above 150 nm (N >150 ). Concurrent balloon-borne meteorological measurements provided context for the continuous profiles through the cloudy atmospheric boundary layer. Radiosoundings, cloud remote sensing data, and 5-day back trajectories supplemented the analysis. The majority of aerosol profiles showed more particles above the lowest temperature inversion, on average, double the number concentration compared to below. Increased N 12−150 up to 3,000 cm −3 were observed in the free troposphere above low-level clouds related to secondary particle formation. Long-range transport of pollution increased N >150 to 310 cm −3 in a warm, moist air mass. Droplet activation inside clouds caused reductions of N >150 by up to 100%, while the decrease in N 12−150 was less than 50%. When low-level clouds were thermodynamically coupled with the surface, profiles showed 5 times higher values of N 12−150 in the free troposphere than below the cloud-capping temperature inversion. Enhanced N 12−150 and N >150 interacting with clouds were advected above the lowest inversion from beyond the sea ice edge when clouds were decoupled from the surface. Vertically discontinuous aerosol profiles below decoupled clouds suggest that particles emitted at the surface are not transported to clouds in these conditions. It is concluded that the cloud-surface coupling state and free tropospheric particle abundance are crucial when assessing the aerosol budget for Arctic low-level clouds over sea ice.

54 ENVIRONMENTAL SCIENCES↗

Enhancements in Cloud Condensation Nuclei Activity From Turbulent Fluctuations in Supersaturation

Abstract The effect of aerosols on the properties of clouds is a large source of uncertainty in predictions of weather and climate. These aerosol‐cloud interactions depend critically on the ability of aerosol particles to form cloud droplets. A challenge in modeling aerosol‐cloud interactions is the representation of interactions between turbulence and cloud microphysics. Turbulent mixing leads to small‐scale fluctuations in water vapor and temperature that are unresolved in large‐scale atmospheric models. To quantify the impact of turbulent fluctuations on cloud condensation nuclei (CCN) activation, we used a high‐resolution Large Eddy Simulation of a convective cloud chamber to drive particle‐based cloud microphysics simulations. We show small‐scale fluctuations strongly impact CCN activity. Once activated, the relatively long timescales of evaporation compared to fluctuations causes droplets to persist in subsaturated regions, which further increases droplet concentrations.

54 ENVIRONMENTAL SCIENCES↗

62°S Witnesses the Transition of Boundary Layer Marine Aerosol Pattern Over the Southern Ocean (50°S–68°S, 63°E– 150°E) During the Spring and Summer: Results From MARCUS (I)

The Atmospheric Radiation Measurement Mobile Facility-2 was installed onboard the research vessel Aurora Australis to measure aerosol properties during the 2017-2018 Measurement of Aerosols, Radiation, and CloUds over the pristine Southern ocean (MARCUS) Experiment, providing unique data on aerosols latitudinal and seasonal variation, including south of 60 degrees S where previous observations are scarce. Data from a Cloud Condensation Nuclei (CCN) counter and Ultra-High-Sensitivity Aerosol Spectrometer show that both the number concentration (N-CCN) and size distribution of CCN-active aerosols, with diameters (D) between 60 nm < D < 1,000 nm are different over the North Southern Ocean (NSO) (50 degrees S-60 degrees S) and the South Southern Ocean (SSO) (62 degrees S-68 degrees S). The average NSO N-CCN at 0.2% and 0.5% supersaturation were 28% and 49% less than that over the SSO. This increase of CCN over the SSO is caused by the increase of aerosols with 60 nm < D < 200 nm, consistent with calculations of Aerosol Scattering Angstrom Exponents derived from a nephelometer. Aerosol hygroscopicity growth factor measured by the Hygroscopic Tandem Differential Mobility Analyzer stayed close to 1.41 for aerosols with 50 nm < D < 250 nm over the SSO, but increased from 1.30 to 1.67 over the NSO, indicating different chemical compositions. Both CCN and Ice Nucleating Particles (INPs) showed a stronger variation with season than with latitude. The variation of heat-labile and presumably proteinacous INPs suggests an increase of ice nucleating-active microbes in summer.

Niu, Qing↗

Metamodeling of Droplet Activation for Global Climate Models

The nucleation of cloud droplets from the ambient aerosol is a critical physical process that must be resolved for global models to faithfully predict aerosol–cloud interactions and aerosol indirect effects on climate. To better represent droplet nucleation from a complex, multimodal, and multicomponent aerosol population within the context of a global model, a new metamodeling framework is applied to derive an efficient and accurate activation parameterization. The framework applies polynomial chaos expansion to a detailed parcel model in order to derive an emulator that maps thermodynamic and aerosol parameters to the supersaturation maximum achieved in an adiabatically ascending parcel and can be used to diagnose droplet number from a single lognormal aerosol mode. The emulator requires much less computational time to build, store, and evaluate than a high-dimensional lookup table. Compared to large sample sets from the detailed parcel model, the relative error in the predicted supersaturation maximum and activated droplet number computed with the best emulator is and (one standard deviation), respectively. On average, the emulators constructed here are as accurate and between 10 and 17 times faster than a leading physically based activation parameterization. Because the underlying parcel model being emulated resolves size-dependent droplet growth factors, the emulator captures kinetic limitations on activation. Furthermore, the results discussed in this work suggest that this metamodeling framework can be extended to accurately account for the detailed activation of a complex aerosol population in an arbitrary coupled global aerosol–climate model.

54 ENVIRONMENTAL SCIENCES↗

Effective radiative forcing and adjustments in CMIP6 models

Abstract. The effective radiative forcing, which includes the instantaneous forcing plus adjustments from the atmosphere and surface, has emerged as the key metric of evaluating human and natural influence on the climate. We evaluate effective radiative forcing and adjustments in 17 contemporary climate models that are participating in the Coupled Model Intercomparison Project (CMIP6) and have contributed to the Radiative Forcing Model Intercomparison Project (RFMIP). Present-day (2014) global-mean anthropogenic forcing relative to pre-industrial (1850) levels from climate models stands at 2.00 (±0.23) W m−2, comprised of 1.81 (±0.09) W m−2 from CO2, 1.08 (± 0.21) W m−2 from other well-mixed greenhouse gases, −1.01 (± 0.23) W m−2 from aerosols and −0.09 (±0.13) W m−2 from land use change. Quoted uncertainties are 1 standard deviation across model best estimates, and 90 % confidence in the reported forcings, due to internal variability, is typically within 0.1 W m−2. The majority of the remaining 0.21 W m−2 is likely to be from ozone. In most cases, the largest contributors to the spread in effective radiative forcing (ERF) is from the instantaneous radiative forcing (IRF) and from cloud responses, particularly aerosol–cloud interactions to aerosol forcing. As determined in previous studies, cancellation of tropospheric and surface adjustments means that the stratospherically adjusted radiative forcing is approximately equal to ERF for greenhouse gas forcing but not for aerosols, and consequentially, not for the anthropogenic total. The spread of aerosol forcing ranges from −0.63 to −1.37 W m−2, exhibiting a less negative mean and narrower range compared to 10 CMIP5 models. The spread in 4×CO2 forcing has also narrowed in CMIP6 compared to 13 CMIP5 models. Aerosol forcing is uncorrelated with climate sensitivity. Therefore, there is no evidence to suggest that the increasing spread in climate sensitivity in CMIP6 models, particularly related to high-sensitivity models, is a consequence of a stronger negative present-day aerosol forcing and little evidence that modelling groups are systematically tuning climate sensitivity or aerosol forcing to recreate observed historical warming.

54 ENVIRONMENTAL SCIENCES↗

Viewing Atmospheric Aerosols from the MODIS Satellite Sensor

The MODerate resolution Imaging Spectroradiometer (MODIS) currently aboard both the Terra and Aqua satellites produces a suite of products designed to characterize global aerosol distribution, optical thickness and particle size. Never before has a space-borne instrument been able to provide such detailed information, complementing field and modeling efforts to produce a comprehensive picture of aerosol characteristics. The three years of Terra-MODIS data have been validated by comparing with co-located AERONET observations of aerosol optical thickness and derivations of aerosol size parameters. Some 8000 comparison points located at 133 AERONET sites around the globe show that the MODIS aerosol optical thickness retrievals are accurate to within the pre-launch expectations, on a global basis. The global statistics, however, can hide local biases in the product. Some of these biases will be discussed. Nevertheless, the products can be used and are currently being used to answer some pressing questions concerning aerosol radiative forcing, aerosol-cloud interaction, estimating aerosol sources and height of transport, and Air Quality forecasting. A survey of current applications of MODIS aerosol products will be presented.

Remer, L.↗

Effective radiative forcing and adjustments in CMIP6 models

The effective radiative forcing, which includes the instantaneous forcing plus adjustments from the atmosphere and surface, has emerged as the key metric of evaluating human and natural influence on the climate. We evaluate effective radiative forcing and adjustments in 17 contemporary climate models that are participating in the Coupled Model Intercomparison Project (CMIP6) and have contributed to the Radiative Forcing Model Intercomparison Project (RFMIP). Present-day (2014) global-mean anthropogenic forcing relative to pre-industrial (1850) levels from climate models stands at 2.00 (±0.23) W/sq. m, comprised of 1.81 (±0.09) W/sq. m from CO2, 1.08 (± 0.21) W/sq. m from other well-mixed greenhouse gases, −1.01 (± 0.23) W/sq. m from aerosols and −0.09 (±0.13) W/sq. m from land use change. Quoted uncertainties are 1 standard deviation across model best estimates, and 90 % confidence in the reported forcings, due to internal variability, is typically within 0.1 W/sq. m. The majority of the remaining 0.21 W/sq. m is likely to be from ozone. In most cases, the largest contributors to the spread in effective radiative forcing (ERF) is from the instantaneous radiative forcing (IRF) and from cloud responses, particularly aerosol–cloud interactions to aerosol forcing. As determined in previous studies, cancellation of tropospheric and surface adjustments means that the stratospherically adjusted radiative forcing is approximately equal to ERF for greenhouse gas forcing but not for aerosols, and consequentially, not for the anthropogenic total. The spread of aerosol forcing ranges from −0.63 to −1.37 W/sq. m, exhibiting a less negative mean and narrower range compared to 10 CMIP5 models. The spread in 4×CO2 forcing has also narrowed in CMIP6 compared to 13 CMIP5 models. Aerosol forcing is uncorrelated with climate sensitivity. Therefore, there is no evidence to suggest that the increasing spread in climate sensitivity in CMIP6 models, particularly related to high-sensitivity models, is a consequence of a stronger negative present-day aerosol forcing and little evidence that modelling groups are systematically tuning climate sensitivity or aerosol forcing to recreate observed historical warming.

effective radiative forcing↗

An Automatic Light Rain Detection Algorithm on NASA MPLNET Lidar Observations in the Frame of WMO GALION Project

The water cycle strongly influences life on Earth. In particular, the precipitation modifies the atmospheric column thermodynamics through the process of evaporation and serves as a proxy for latent heat modulation. For this reason, a correct precipitation parameterization (especially low-intensity precipitation) at global scale, bedsides improving our understanding of the hydrological cycle, it is crucial to reduce the associated uncertainty of the global climate models to correctly forecast future scenarios, i.e. to apply fast mitigation strategies. In this study we developed an algorithm to automatically detect precipitation from lidar measurements obtained by the National and Aeronautics Space Administration (NASA) Micropulse lidar network (MPLNET) permanent observational site in Goddard. The algorithm, once full operational, will deliver in Near Real Time (latency 1.5h) a new rain mask product that will be publicly available on MPLNET website as part of the new Version 3 Level 1.5 data. The methodology, based on an image processing technique, can detect only light precipitation events (defined by intensity and duration) as the morphological filters used through the detection process are applied on the lidar volume depolarization ratio range corrected composite images, i.e. heavy rain events are unusable as the lidar signal is completely extinguished after few meters in the precipitation or no signal detected because of the water accumulated on the receiver optics. Results from the algorithm, besides filling a gap in precipitation and virga detection by radars, are of particular interest for the scientific community because will help to better understand long-term aerosol-cloud interactions and aerosol atmospheric removal (scavenging effect) by rain as multi-year database being available for several MPLNET permanent observational sites across the globe. Moreover, we developed the automatic algorithm at Universitat Politecnica de Catalunya (UPC) Barcelona, the unique permanent observation station member of MPLNET and the European Aerosol Lidar Network (EARLINET) In the future the algorithm can be then easily applied to any other lidar and/or ceilometer network infrastructure in the frame of World Meteorological Organization (WMO) Global Aerosol Watch (GAW) aerosol lidar observation network (GALION)

Simone Lolli↗

Scattering and Absorbing Aerosols in the Climate System

Tropospheric anthropogenic aerosols contribute the second-largest forcing to climate change, but with high uncertainty owing to their spatio-temporal variability and complicated optical properties. In this Review, we synthesize understanding of aerosol observations and their radiative and climate effects. Aerosols offset about one-third of the warming effect by anthropogenic greenhouse gases. Yet, in regions and seasons where the absorbing aerosol fraction is high — such as South America and East and South Asia — substantial atmospheric warming can occur. The internal mixing and the vertical distribution of aerosols, which alters both the direct effect and aerosol–cloud interactions, might further enhance this warming. Despite extensive research in aerosol–cloud interactions, there is still at least a 50% spread in total aerosol forcing estimates. This ongoing uncertainty is linked, in part, to the poor measurement of anthropogenic and natural aerosol absorption, as well as the little-understood effects of aerosols on clouds. Next-generation, space-borne, multi-angle polarization and active remote sensing, combined with in situ observations, offer opportunities to better constrain aerosol scattering, absorption and size distribution, thus, improving models to refine estimates of aerosol forcing and climate effects.

Tropospheric anthropogenic aerosols↗

A Model Intercomparison Study of Aerosol‐Cloud‐Turbulence Interactions in a Cloud Chamber: 1. Model Results

This study presents the first model intercomparison of aerosol‐cloud‐turbulence interactions in a controlled cloudy Rayleigh‐Bénard Convection chamber environment, utilizing the Pi Chamber at Michigan Technological University. We analyzed simulated cloud chamber‐averaged statistics of microphysics and thermodynamics in a warm‐phase, cloudy environment under steady‐state conditions at varying aerosol injection rates. Simulation results from seven distinct models (DNS, LES, and a 1D turbulence model) were compared. Our findings demonstrate that while all models qualitatively capture observed trends in droplet number concentration, mean radius, and droplet size distributions at both high and low aerosol injection rates, significant quantitative differences were observed. Notably, droplet number concentrations varied by over two orders of magnitude between models for the same injection rates, indicating sensitivities to the model treatments in droplet activation and removal and wall fluxes. Furthermore, inconsistencies in vertical relative humidity profiles and in achieving steady‐state liquid water content suggest the need for further investigation into the mechanisms driving these variations. Despite these discrepancies, the models generally reproduced consistent power‐law relationships between the microphysical variables. This model intercomparison underscores the importance of controlled cloud chamber experiments for validating and improving cloud microphysical parameterizations. Recommendations for future modeling studies are also highlighted, including constraining wall conditions and processes, investigating droplet/aerosol removal (including sidewall losses), and conducting simplified experiments to isolate specific processes contributing to model divergence and reduce model uncertainties.

54 ENVIRONMENTAL SCIENCES↗