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At least 145 records · Page 8

Radiative Forcing of Nitrate Aerosols From 1975 to 2010 as Simulated by MOSAIC Module in CESM2-MAM4

In this work, we incorporate the Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) module in the Community Earth System Model version 2 (CESM2) Community Atmosphere Model Version 6 with interactive chemistry (CAM6-chem), and couple it with the four mode version of the Modal Aerosol Module (MAM4). The MOSAIC module is used to simulate the thermodynamics of the gas-aerosol mass exchange, with a special focus on simulating nitrate aerosol. By comparing against ground and satellite observations, we found that the MOSAIC/MAM4 scheme performs reasonably well in simulating spatiotemporal distributions of aerosols, including nitrate aerosol. We conducted a series of model experiments with and without nitrate aerosols, and examined the radiative effect (RE) associated with nitrate aerosols in 1975, 2000, and 2010, and accessed the radiative forcing (RF) of nitrate aerosols between the present day and pre-industrial periods. Comparing with the nitrate aerosol RE, we predicted relatively small RF of anthropogenic nitrate aerosol from aerosol-radiation interactions (RF ari : -0.014 W m -2 ) and large RF from aerosol-cloud interactions (RF aci : -0.219 W m -2 ). Regional signatures of nitrate RE/RF are noticeable and important: for instance, very small changes in RE ari in Europe and USA, but 2.8–3 times increases in RE ari in India and China from 1975 to 2010, while RE aci /RF aci in China is a warming effect due to the competing effect between sulfate and nitrate aerosols as cloud condensation nuclei.

54 ENVIRONMENTAL SCIENCES↗

A single-photon lidar observes atmospheric clouds at decimeter scales: resolving droplet activation within cloud base

Abstract Clouds, crucial for understanding climate, begin with droplet formation from aerosols, but observations of this fleeting activation step are lacking in the atmosphere. Here we use a time-gated time-correlated single-photon counting lidar to observe cloud base structures at decimeter scales. Results show that the air–cloud interface is not a perfect boundary but rather a transition zone where the transformation of aerosol particles into cloud droplets occurs. The observed distributions of first-arriving photons within the transition zone reflect vertical development of a cloud, including droplet activation and condensational growth. Further, the highly resolved vertical profile of backscattered photons above the cloud base enables remote estimation of droplet concentration, an elusive but critical property to understanding aerosol–cloud interactions. Our results show the feasibility of remotely monitoring cloud properties at submeter scales, thus providing much-needed insights into the impacts of atmospheric pollution on clouds and aerosol-cloud interactions that influence climate.

54 ENVIRONMENTAL SCIENCES↗

Do Arctic mixed-phase clouds sometimes dissipate due to insufficient aerosol? Evidence from comparisons between observations and idealized simulations

Abstract. Mixed-phase clouds are ubiquitous in the Arctic. These clouds can persist for days and dissipate in a matter of hours. It is sometimes unknown what causes this sudden dissipation, but aerosol–cloud interactions may be involved. Arctic aerosol concentrations can be low enough to affect cloud formation and structure, and it has been hypothesized that, in some instances, concentrations can drop below some critical value needed to maintain a cloud. We use observations from a Department of Energy ARM site on the northern slope of Alaska at Oliktok Point (OLI), the Arctic Summer Cloud Ocean Study (ASCOS) field campaign in the high Arctic Ocean, and the Integrated Characterisation of Energy, Clouds, Atmospheric state, and Precipitation at Summit – Aerosol Cloud Experiment (ICECAPS-ACE) project at the NSF (National Science Foundation) Summit Station in Greenland (SMT) to identify one case per site where Arctic boundary layer clouds dissipated coincidentally with a decrease in surface aerosol concentrations. These cases are used to initialize idealized large eddy simulations (LESs) in which aerosol concentrations are held constant until, at a specified time, all aerosols are removed instantaneously – effectively creating an extreme case of aerosol-limited dissipation which represents the fastest a cloud could possibly dissipate via this process. These LESs are compared against the observed data to determine whether cases could, potentially, be dissipating due to insufficient aerosol. The OLI case's observed liquid water path (LWP) dissipated faster than its simulation, indicating that other processes are likely the primary drivers of the dissipation. The ASCOS and SMT observed LWP dissipated at similar rates to their respective simulations, suggesting that aerosol-limited dissipation may be occurring in these instances. We also find that the microphysical response to this extreme aerosol forcing depends greatly on the specific case being simulated. Cases with drizzling liquid layers are simulated to dissipate by accelerating precipitation when aerosol is removed while the case with a non-drizzling liquid layer dissipates quickly, possibly glaciating via the Wegener–Bergeron–Findeisen (WBF) process. The non-drizzling case is also more sensitive to ice-nucleating particle (INP) concentrations than the drizzling cases. Overall, the simulations suggest that aerosol-limited cloud dissipation in the Arctic is plausible and that there are at least two microphysical pathways by which aerosol-limited dissipation can occur.

54 ENVIRONMENTAL SCIENCES↗

Final report: Insights from ARM observations into aerosol processing and transport by extratropical cyclones and aerosol effects on cyclone clouds

This project advanced understanding of aerosol–cloud interactions in extratropical cyclones using observations from the Atmospheric Radiation Measurement (ARM) Eastern North Atlantic (ENA) observatory and ACE-ENA field campaigns, along with satellite datasets and numerical modeling. We have quantified the susceptibility of frontal clouds to aerosols, showing that this susceptibility is similar to that in non-frontal clouds despite substantial (factor 2) differences in droplet concentrations between these cloud types, and also significant differences in cloud albedo. A key finding was that Aitken-mode (here, 60-100nm diameter) aerosols play a disproportionately important role in droplet activation in frontal clouds, and concentrations of these particles are frequently strongly biased in climate models. Activation of aerosols depends strongly on updraft speeds, and via collaboration with Argonne National Laboratory we contributed to quantifying these better with the ARM radar wind profiler at the ENA site. Our studies in the North Atlantic have analogs in the Southern Ocean, and to draw these out we examined data from the MARCUS and SOCRATES field campaigns. We identified new particle formation within extratropical cyclones as a potentially important source of cloud condensation nuclei in these pristine marine environments. By combining ARM observations with perturbed parameter ensemble simulations, we demonstrated that surface observations can effectively constrain aerosol–cloud adjustments and reduce uncertainty in simulated cloud liquid water path responses by approximately 15%, yielding stronger constraints on historical aerosol cooling effects. The work further established precipitation processes as a dominant control on aerosol–cloud interactions and Earth system predictability.

Gordon, Hamish [Department of Chemical Engineering↗

Cloud–Aerosol–Turbulence Interactions: Science Priorities and Concepts for a Large-Scale Laboratory Facility

The purpose of this meeting summary, therefore, is to outline the range of scientific questions, and the facility concepts that were explored.We began the workshop with a series of overview talks to highlight scientific questions that could be investigated in a large-scale aerosol-cloud-turbulence laboratory facility. Topics included warm and mixed-phase cloud microphysics, aerosol and cloud chemistry, atmospheric turbulence, radiative transfer, cloud/aerosol instrumentation, and remote sensing. There was ample time for questions and discussion following each overview presentation. We also broke into groups for several hours at various points to enable more active discussion among all participants.

54 ENVIRONMENTAL SCIENCES↗

The ATTO-Campina site: A new observatory for tropical convection and gas-aerosol-cloud-precipitation interactions in the Amazon

We present results from ATTO-Campina, a new permanent observational site in central Amazon, about 4 km from the ATTO towers. Operational since 2020, ATTO-Campina characterizes atmospheric, cloud and rainfall properties through remote sensing. The goal is to provide continuous, complementary measurements to the ATTO towers, addressing the rainforest’s complex gas-aerosol-cloud-precipitation dynamics. Using a 3.5-year dataset, we classified convective clouds into three types: shallow cumulus (ShCu), congestus (Con) or (Deep) clouds. The shallow-to-deep transition takes about three hours, starting with ShCu formation at 11:00 local time. The accumulated rainfall peak follows at about 16:00. Only weak downdrafts are present in the upper troposphere where previous studies indicate new particle formation (NPF) occurrence. Strong downdrafts are mostly limited to heights below 5 km. Con and Deep convective days have higher concentrations of ultrafine aerosol and lower concentrations of accumulation-mode particles compared to ShCu. Convective clouds also significantly modify gas mixing ratios. Deep convective clouds are associated with high near-surface O3, consistent with downward transport from the midtroposphere. Our results showcase the added detail achieved by integrating data from the ATTO towers and ATTO-Campina sites. Together, these sites support better understanding of interconnected gas-aerosol-cloud-precipitation processes in the Amazon and their evolution under climate change.

54 ENVIRONMENTAL SCIENCES↗

Open cells exhibit weaker entrainment of free-tropospheric biomass burning aerosol into the south-east Atlantic boundary layer

This work presents synergistic satellite, airborne and surface-based observations of a pocket of open cells (POC) in the remote south-east Atlantic. The observations were obtained over and upwind of Ascension Island during the CLouds and Aerosol Radiative Impacts and Forcing (CLARIFY) and the Layered Smoke Interacting with Clouds (LASIC) field experiments. A novel aspect of this case study is that an extensive free-tropospheric biomass burning aerosol plume that had been transported from the African continent was observed to be in contact with the boundary layer inversion over the POC and the surrounding closed cellular cloud regime. The in situ measurements show marked contrasts in the boundary layer thermodynamic structure, cloud properties, precipitation and aerosol conditions between the open cells and surrounding overcast cloud field. The data demonstrate that the overlying biomass burning aerosol was mixing down into the boundary layer in the stratocumulus cloud downwind of the POC, with elevated carbon monoxide, black carbon mass loadings and accumulation-mode aerosol concentrations measured beneath the trade-wind inversion. The stratocumulus cloud in this region was moderately polluted and exhibited very little precipitation falling below cloud base. A rapid transition to actively precipitating cumulus clouds and detrained stratiform remnants in the form of thin quiescent veil clouds was observed across the boundary into and deep within the POC. The subcloud layer in the POC was much cleaner than that in the stratocumulus region. The clouds in the POC formed within an ultra-clean layer (accumulation-mode aerosol concentrations of approximately a few cm -3 ) in the upper region of the boundary layer, which was likely to have been formed via efficient collision–coalescence and sedimentation processes. Enhanced Aitken-mode aerosol concentrations were also observed intermittently in this ultra-clean layer, suggesting that new particle formation was taking place. Across the boundary layer inversion and immediately above the ultra-clean layer, accumulation-mode aerosol concentrations were ~1000 cm -3 . Importantly, the air mass in the POC showed no evidence of elevated carbon monoxide over and above typical background conditions at this location and time of year. As carbon monoxide is a good tracer for biomass burning aerosol that is not readily removed by cloud processing and precipitation, it demonstrates that the open cellular convection in the POC is not able to entrain large quantities of the free-tropospheric aerosol that was sitting directly on top of the boundary layer inversion. This suggests that the structure of the mesoscale cellular convection may play an important role in regulating the transport of aerosol from the free troposphere down into the marine boundary layer. We then develop a climatology of open cellular cloud conditions in the south-east Atlantic from 19 years of September Moderate Resolution Imaging Spectroradiometer (MODIS) Terra imagery. This shows that the maxima in open cell frequency (> 0.25) occurs far offshore and in a region where subsiding biomass burning aerosol plumes may often come into contact with the underlying boundary layer cloud. If the results from the observational case study applied more broadly, then the apparent low susceptibility of open cells to free-tropospheric intrusions of additional cloud condensation nuclei could have some important consequences for aerosol–cloud interactions in the region.

54 ENVIRONMENTAL SCIENCES↗

Size-resolved Eddy-Covariance Particle Flux Measurement during the TRACER Campaign (Final Report)

The main goal of the TRacking Aerosol Convection interactions ExpeRiment (TRACER) campaign was to study aerosol–cloud interactions during deep convection over the Houston area. This project deployed a suite of instrumentation with the aim to (1) quantify turbulent vertical particle fluxes during at DOE-ARM sites, including TRACER, (2) assess hygroscopic growth factors and hygroscopicity parameters of the material driving modal aerosol growth during new particle formation and growth events, (3) derive turbulent aerosol mass fluxes using co-located Doppler LIDAR measurements, and (4) create quality-controlled PI data products to support future research utilizing data collected during the TRACER campaign. This report summarized the main findings from the deployments at two DOE-ARM sites. Briefly, we found that new particle formation may occur aloft, in a residual layer, near the top of the boundary layer. Small grown particles appear later due to downward mixing with daytime turbulence. The species that are responsible for aerosol modal growth had hygroscopicity parameters varying between 0.05 and 0.34. These values systematically depended on the wind sector, suggesting that the chemical composition of the precursors differed. This work demonstrated that lidar retrievals of the elastic backscatter and Doppler velocity can be used to obtain surface number emissions of particles with a diameter greater than 0.53 µm. During TRACER, emission particle number fluxes peaked near ∼ 100 cm−2 s−1. Multiple quality-controlled PI data products that will support future TRACER related science were generated and made publically available.

54 ENVIRONMENTAL SCIENCES↗

Features of mid- and high-latitude low-level clouds and their relation to strong aerosol effects in the Energy Exascale Earth System Model version 2 (E3SMv2)

The E3SMv2 model, like various other global models that include representations of aerosol–cloud interactions, uses an empirically chosen lower bound on the simulated in-cloud cloud droplet number concentration (CDNC) to help constrain the effective radiative forcing of anthropogenic aerosols, ERFaer. This study identifies where ultra-low CDNCs (i.e., concentrations lower than 10 cm−3) occur in the stratiform and shallow convective clouds simulated by E3SMv2 and which of the occurrences have the strongest impact on ERF aer . Process-level analyses are presented to reveal characteristics of the cloud droplet formation and removal processes associated with impactful ultra-low CDNCs. Simulations performed with present-day emissions show that ultra-low CDNCs are most frequently found over the mid- and high-latitude oceans in both hemispheres, while the occurrences are also frequent in polluted continental regions despite the high aerosol concentrations. Ultra-low CDNCs with the largest impacts on the simulated regional and global mean ERF aer are found in the lower troposphere in the Northern Hemisphere middle and high latitudes. These cases are typically associated with large cloud fractions, strong water vapor condensation, weak turbulence, and lack of cloud droplet nucleation from aerosol activation. Under such atmospheric conditions, boosting aerosol activation and enhancing turbulent mixing of cloud droplet number can increase the simulated CDNCs, although the magnitude of the global mean ERF aer increases undesirably. The reason for this model behavior is discussed. Overall, our study suggests that mid- and high-latitude low-level stratus occurring under weak turbulence is a cloud regime worth further investigating for the purpose of identifying and addressing the root causes of ultra-low CDNCs and strong ERF aer in E3SM.

Aerosol-Cloud Interaction↗

Biological enhancement of cloud droplet concentrations observed off East Antarctica

Abstract The impact that biogenic emissions have on aerosol-cloud interactions across the Southern Ocean is poorly quantified. Here we use satellite and ship observations during austral summer to study these interactions. We present observational evidence that biogenic aerosols increase cloud condensation nuclei and cloud droplet number concentrations over the Southern Ocean off East Antarctica, coinciding with very low concentrations of ice-nucleating particles and higher occurrences of supercooled liquid-containing low-level clouds.

Mallet, Marc D.↗

Marine Shallow Cloud Adjustments to the Presence of Shortwave-Absorbing Aerosols: Advancing Understanding Through a Combined Analysis of Lasic Datasets and Process Modeling (Final Report)

This is a final report for this award, whose purpose was to support the analysis of data emanating from the LASIC (Layered Atlantic Smoke Interaction with Clouds) campaign. (Layered Atlantic Smoke Interactions with Clouds) is a strategy to improve our understanding of aged carbonaceous aerosol, its seasonal evolution, and the mechanisms by which clouds adjust to the presence of the aerosol. The observational strategy centers on deploying the AMF1 cloud, aerosol, and atmospheric profiling instrumentation to Ascension Island, located within the trade-wind shallow cumulus regime (14.50W, 80S) 3000 km offshore of continental Africa. The location is within the latitude zone of the maximum outflow of aerosol, with the deepening boundary layer known to entrain free-tropospheric smoke. The primary activities for LASIC are: 1) to improve current knowledge on aged biomass burning aerosol and its radiative properties as a function of the seasonal cycle; 2) to use surface-based remote sensing to sensitively interrogate the atmosphere for the relative vertical location of aerosol and clouds; 3) to improve our understanding of the cloud adjustments to the presence of shortwave-absorbing aerosol within the vertical column, both through aerosol-radiation and through aerosol-cloud interactions; 4) to aid low cloud parameterization efforts for climate models. This award serves to further these activities and includes a sub-award to Dr. Pablo Saide at UCLA for activities 3) and 4).

54 ENVIRONMENTAL SCIENCES↗

Multiscale ACI Satellite Database

The SATELLITE_EAGLES_PNNL NetCDF dataset contains a suite of satellite- and reanalysis-derived atmospheric and surface parameters on a regular latitude–longitude grid. The dataset includes core geophysical fields such as land fraction, aerosol optical depth at multiple wavelengths (465, 550, 667, and 865 nm), sea surface temperature, estimated inversion strength, and various thermodynamic and dynamic quantities (e.g., relative humidity, vertical velocity, boundary-layer height, and surface fluxes) from both MERRA and ERA reanalysis products, provided as daily-mean and instantaneous values. A major component of the dataset consists of MODIS-retrieved cloud microphysical properties, including cloud droplet number concentration, cloud effective radius, optical thickness, and liquid water path, provided for three compositing regimes (“All,” “Q06,” and “G18”). Corresponding cloud-top parameters—temperature, height, and pressure—along with total and domain-mean cloud fraction fields are also included. The file further integrates additional satellite data from AMSR-E (for cloud water, rain water, and surface precipitation retrievals) and CERES (for top-of-atmosphere radiative fluxes, cloud fractions, and albedo). This dataset is designed to evaluate aerosol–cloud interactions in warm clouds, emphasizing the use of MODIS for deriving cloud droplet number concentration and liquid water path statistics. The complementary satellite and reanalysis fields are co-located and time-matched to the same instantaneous MODIS observations, enabling consistent comparisons between cloud properties, aerosol loading, and large-scale meteorological conditions. The dataset is recently featured in Christensen et al. (2025), Machine Learning Reveals Strong Grid-Scale Dependence in the Satellite Nd–LWP Relationship, EGUsphere [preprint], https://doi.org/10.5194/egusphere-2025-3850, 2025.

54 ENVIRONMENTAL SCIENCES↗

Characterizing Greater Houston's Aerosol by Air Mass During TRACER

During the TRacking Aerosol and Convection interaction ExpeRiment (TRACER), a suite of aerosol and cloud measurements were made using the Texas A&M Rapid Onsite Atmospheric Measurement Van (ROAM-V) mobile instrument platform. Joint ROAM-V/radiosonde deployments focused on sampling polluted marine and continental air masses to understand summertime convection along and across the sea-breeze front as it propagated through Houston. The polluted marine air mass at Seawolf Park, Galveston, TX was defined by two characteristic aerosol populations. Although the background total particle concentrations averaged 2,500 cm −3 , the air mass was also influenced by frequent but irregular periods of ship emission with significantly higher aerosol concentrations at times exceeding 34,000 cm −3 . Ship emission influenced periods, typically lasting <10 min, contained smaller, less hygroscopic particles resulting in a 69% relative decline in cloud condensation nuclei (CCN) activated fraction at 1% supersaturation compared to background periods. Measurements in continental air masses northwest of Houston revealed an average aerosol concentration of 5,208 cm −3 with a κ value near 0.1 reasonably describing the CCN population, independent of particle size. In continental air masses, substantial differences in particle size and CCN activation over small distances (<42 miles between sites) suggest considerable site-to-site variability in addition to the expected day-to-day differences. This small-scale variability makes it difficult to generalize continental air mass aerosol properties. Both coastal and inland locations had effective ice nucleating particles, but inland deployments observed the warmest nucleation temperature at −15.6°C compared to −17.8°C close to the coast. These measurements can reduce uncertainties in regional convection allowing models to improve understanding of aerosol-cloud interactions.

54 ENVIRONMENTAL SCIENCES↗

Sensitivity of aerosol optical properties to the aerosol size distribution over central Europe and the Mediterranean Basin using the WRF-Chem v.3.9.1.1 coupled model

The size distribution of atmospheric aerosols plays a key role for understanding and quantifying the uncertainties related to aerosol–radiation and aerosol–cloud interactions. These interactions ultimately depend on the size distribution through optical properties (such as aerosol optical depth, AOD) or cloud microphysical properties. Hence, the main objective of this contribution is to disentangle the impact of the representation of aerosol size distribution on aerosol optical properties over central Europe, particularly over the Mediterranean Basin, during a summertime aerosol episode. To fulfill this objective, a sensitivity test has been conducted using the coupled chemistry–meteorology model WRF-Chem (Weather Research Forecast model coupled with Chemistry). The test modified the parameters defining a lognormal size distribution (geometric diameter and standard deviation) by 10 %, 20 %, and 50 %. Results reveal that the reduction in the standard deviation of the accumulation mode leads to the largest impacts on AOD due to a transfer of particles from the accumulation mode to the coarse mode. A reduction in the geometric diameter of the accumulation mode also has an influence on AOD representation since particles in this mode are assumed to be smaller. In addition, an increase in the geometric diameter of the coarse mode produces a redistribution through the total size distribution by relocating particles from the finer modes to the coarse.

54 ENVIRONMENTAL SCIENCES↗

Larger Cloud Liquid Water Enhances Both Aerosol Indirect Forcing and Cloud Radiative Feedback in Two Earth System Models

Previous studies have noticed that the Coupled Model Intercomparison Project Phase 6 (CMIP6) models with a stronger cooling from aerosol-cloud interactions (ACI) also have an enhanced warming from positive cloud feedback, and these two opposing effects are counter-balanced in simulations of the historical period. However, reasons for this anti-correlation are less explored. In this study, we perturb the cloud ice microphysical processes to obtain cloud liquid of varying amounts in two Earth System Models (ESMs). We find that the model simulations with a larger liquid water path (LWP) tend to have a stronger cooling from ACI and a stronger positive cloud feedback. More liquid clouds in the mean-state present more opportunities for anthropogenic aerosol perturbations and also weaken the negative cloud feedback at middle to high latitudes. This work, from a cloud state perspective, emphasizes the influence of the mean-state LWP on effective radiative forcing due to ACI (ERF ACI ).

54 ENVIRONMENTAL SCIENCES↗

Aerosol effective radiative forcing increases Earth’s energy imbalance in recent decades

Earth’s energy imbalance (EEI), a key driver of climate change, has risen markedly over the last two decades. Greenhouse gas forcing, aerosol forcing, and cloud feedback all contribute to this increase. However, the role of aerosol forcing, particularly effective radiative forcing through aerosol-cloud interactions (ERF ACI ), remains highly uncertain and closely intertwined with cloud feedback. Here, we estimate shortwave ERF ACI using satellite observations and show its importance as a contributor to the EEI increase between 2003 and 2023. ERF ACI exhibits a significant increasing trend of 0.33 Wm −2 /decade averaged over oceans between 60°S and 60°N. The increasing trend of ERF ACI stems from a global decline in cloud droplet number concentration driven by decreasing anthropogenic aerosol emissions. It is of similar magnitude as the combined instantaneous forcing trend from greenhouse gases and aerosol-radiation interactions. Our results may reduce the gap between the simulated and observed shortwave contribution to EEI trends while implying a weak shortwave cloud feedback. They also suggest a stronger aerosol forcing than the multi-model mean.

Yuan, Tianle [NASA Goddard Space Flight Center (GS↗