SEARCH · Search NASA

Results for “Aerosol cloud interactions”

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

SourceResearch connectionFrom yearThrough year

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

At least 199 records · Page 11

All sources NASA NTRS DOE OSTI

DOE OSTI2025

Advancing the Understanding of Cloud Microphysical Processes and Aerosol Indirect Effects in High-Latitude Mixed-Phase Clouds by Linking ARM Measurements with Climate Model Simulations (Final Report)

The key objectives of this project were to advance our understanding of cloud microphysical characteristics and aerosol indirect effects on mixed-phase clouds in high latitudes. To improve the representation of ice and mixed-phase clouds in Earth System Models (ESMs), we propose an integrated observation and modeling study of cloud macro- and microphysical properties, including spatial heterogeneities, mass partitioning between ice crystals and supercooled liquid water, effects of ice nucleating particles (INPs), and efficiency of secondary ice production (SIP), etc. Specifically, we took four main approaches in this project: (1) examining macro- and microphysical properties of ice and mixed-phase clouds based on in-situ and ground-based observations from multiple field campaigns funded by the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) program, including the Mixed-Phase Arctic Cloud Experiment (M-PACE), Indirect and Semi-Direct Aerosol Campaign (ISDAC), Ice Nucleating Particle Sources at Oliktok Point (INPOP), ARM West Antarctic Radiation Experiment (AWARE), Measurements of Aerosols, Radiation, and Clouds over the Southern Ocean (MARCUS), and Macquarie Island Cloud and Radiation Experiment (MICRE); (2) evaluating the DOE Energy Exascale Earth System Model (E3SM) simulations based on observations, particularly for ice and mixed-phase cloud microphysical properties; (3) examining the impacts of INPs on ice and mixed-phase clouds. Specifically, a series of comparisons were conducted using observations over the Arctic, Southern Ocean, and Antarctica, including comparisons between the lower and higher southern latitudes as well as comparisons between the northern and southern hemispheres. In addition, aerosol indirect effects from distinct sources of dust particles were examined; and (4) investigating the impacts of SIP. Ultimately, these results helped to improve cloud microphysics and aerosol-cloud interaction parameterizations in the E3SM model. Overall, the project provided improved understanding regarding various factors, including thermodynamic, dynamic, and aerosol conditions, on the micro- and macrophysical properties of ice and mixed-phase clouds in the high latitudes. Resulting analysis helped to provide an improved physical basis for refining the current cloud microphysics parameterizations related to ice and mixed-phase clouds in E3SM.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Drivers of Cloud Condensation Nuclei in the Eastern North Atlantic as Observed at the ARM Site

Abstract Seven years of data collected at the Atmospheric Radiation Measurement's Eastern North Atlantic (ENA) site are analyzed to understand the controls of Cloud Condensation Nuclei (CCN) concentrations in the region. Day‐night differences in the aerosol data as segregated by wind direction demonstrate the aerosol observations to be impacted by local emissions when the wind direction (wdir) is between 90° and 310° (measured clockwise from the North where air is coming from). Data collected during marine conditions (wdir <90° or wdir >310°) show the CCN concentrations to be higher in the summer months as compared to the winter months. CCN budget analysis revealed advection and precipitation scavenging being primarily responsible for modulating the CCN concentrations at the site on monthly timescales, with rain rates driving the precipitation scavenging term. High (greater than 75th percentile) and low (lower than 25th percentile) CCN events were identified for each month to characterize the sub‐monthly variability of CCN concentrations. Low CCN events had thicker clouds, stronger rain rates, and lower reanalysis reported free‐tropospheric aerosol pseudo number concentration at the ENA site as compared to the high CCN events. Analysis of satellite data of air‐parcels 48 hr prior to their arrival at the ENA site demonstrated the air parcels during low CCN events to encounter higher cloudiness, stronger rain rates, and higher cloud top heights as compared to the high CCN events. The results presented herein provide key constraints for model evaluation studies and climatological studies conducted at the ENA site.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Identifying a regional aerosol baseline in the eastern North Atlantic using collocated measurements and a mathematical algorithm to mask high-submicron-number-concentration aerosol events

Abstract. High-time-resolution measurements of in situ aerosol and cloud properties provide the ability to study regional atmospheric processes that occur on timescales of minutes to hours. However, one limitation to this approach is that continuous measurements often include periods when the data collected are not representative of the regional aerosol. Even at remote locations, submicron aerosols are pervasive in the ambient atmosphere with many sources. Therefore, periods dominated by local aerosol should be identified before conducting subsequent analyses to understand aerosol regional processes and aerosol–cloud interactions. Here, we present a novel method to validate the identification of regional baseline aerosol data by applying a mathematical algorithm to the data collected at the U.S. Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) user facility in the eastern North Atlantic (ENA). The ENA central facility (C1) includes an aerosol observing system (AOS) for the measurement of aerosol physical, optical, and chemical properties at time resolutions from seconds to minutes. A second temporary supplementary facility (S1), located ∼0.75 km from C1, was deployed for ∼1 year during the Aerosol and Cloud Experiments (ACE-ENA) campaign in 2017. First, we investigate the local aerosol at both locations. We associate periods of high submicron number concentration (Ntot) in the fine-mode condensation particle counter (CPC) and size distributions from the Ultra-High Sensitivity Aerosol Spectrometer (UHSAS) as a function of wind direction using a meteorology sensor with local sources. Elevated concentrations of Aitken-mode (< 100 nm diameter) particles were observed in correspondence with the wind directions associated with airport operations. At ENA, the Graciosa Airport and its associated activities were found to be the main sources of high-concentration aerosol events at ENA, causing peaks in 1 min Ntot that exceeded 8000 and 10 000 cm−3 at C1, in summer and winter, respectively, and 5000 cm−3 at S1 in summer. Periods with high Ntot not associated with these wind directions were also observed. As a result, the diverse local sources at ENA yielded a poor relationship between Ntot measurements collected at C1 and S1 (R2=0.03 with a slope =0.05±0.001). As a first approach to mask these events, the time periods when the wind direction was associated with the airport operations (west to northwest and southeast to south at C1 and east to south at S1) were applied. The meteorological masks removed 38.9 % of the data at C1 and 43.4 % at S1, and they did not significantly improve the relationship between the two sites (R2=0.18 with a slope =0.06±0.001). Due to the complexity of high-Ntot events observed at ENA, we develop and validate a mathematical ENA Aerosol Mask (ENA-AM) to identify high-Ntot events using 1 min resolution data from the AOS CPC at C1 and S1. After its parameterization and application, ENA-AM generated a high correlation between Ntot in the summer at C1 and S1 (R2=0.87 with a slope =0.84±0.001). We identified the regional baseline at ENA to be 428±228 cm−3 in the summer and 346±223 cm−3 in the winter. Lastly, we compared masked measurements from the AOS with the ARM Aerial Facility (AAF) during flights over C1 in the summer to understand submicron aerosol vertical mixing over C1. The high correlation (R2=0.71 with a slope of 1.04±0.01) observed between C1 and the AAF Ntot collected within an area of 10 km surrounding ENA and at altitudes < 500 m indicated that the submicron aerosol at ENA was well mixed within the first 500 m of the marine boundary layer during the month of July during ACE-ENA. Our novel method for determining a regional aerosol baseline at ENA can be applied to other time periods and at other locations with validation by a secondary site or additional collocated measurements.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Evaluation of four ground-based retrievals of cloud droplet number concentration in marine stratocumulus with aircraft in situ measurements

Abstract. Cloud droplet number concentration (Nd) is crucial for understanding aerosol–cloud interactions (ACI) and associated radiative effects. We present evaluations of four ground-based Nd retrievals based on comprehensive datasets from the Atmospheric Radiation Measurement (ARM) Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) field campaign. The Nd retrieval methods use ARM ENA observatory ground-based remote sensing observations from a micropulse lidar, Raman lidar, cloud radar, and the ARM NDROP (Droplet Number Concentration) value-added product (VAP), all of which also retrieve cloud effective radius (re). The retrievals are compared against aircraft measurements from the fast cloud droplet probe (FCDP) and the cloud and aerosol spectrometer (CAS) obtained from low-level marine boundary layer clouds on 12 flight days during summer and winter seasons. Additionally, the in situ measurements are used to validate the assumptions and characterizations used in the retrieval algorithms. Statistical comparisons of the probability distribution function (PDF) of the Nd and cloud re retrievals with aircraft measurements demonstrate that these retrievals align well with in situ measurements for overcast clouds, but they may substantially differ for broken clouds or clouds with low liquid water path (LWP). The retrievals are applied to 4 years of ground-based remote sensing measurements of overcast marine boundary layer clouds at the ARM ENA observatory to find that Nd (re) values exhibit seasonal variations, with higher (lower) values during the summer season and lower (higher) values during the winter season. The ensemble of various retrievals using different measurements and retrieval algorithms such as those in this paper can help to quantify Nd retrieval uncertainties and identify reliable Nd retrieval scenarios. Of the retrieval methods, we recommend using the micropulse lidar-based method. This method has good agreement with in situ measurements, less sensitivity to issues arising from precipitation and low cloud LWP and/or optical depth, and broad applicability by functioning for both daytime and nighttime conditions.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Assessing modifications to the Abdul-Razzak and Ghan aerosol activation parameterization (version ARG2000) to improve simulated aerosol–cloud radiative effects in the UK Met Office Unified Model (UM version 13.0)

The representation of aerosol activation is a key source of uncertainty in global composition-climate model simulations of aerosol–cloud interactions. The Abdul-Razzak and Ghan (ARG) activation parameterization is used in several global and regional models that employ modal aerosol microphysics schemes. In this study, we investigate the ability of the ARG parameterization to reproduce simulations with a cloud parcel model and find its performance is sensitive to the geometric standard deviations (widths) of the lognormal aerosol modes. We recommend adjustments to three constant parameters in the ARG equations, which improve the performance of the parameterization for small mode widths and its ability to simulate activation in polluted conditions. For the accumulation mode width of 1.4 used in the Met Office Unified Model (UM), the modifications decrease the mean bias in the activated fraction of aerosols compared to a cloud parcel model from −6.6 % to +1.2 %. We implemented the improvements in the UM and compared simulated global cloud droplet concentrations with satellite observations. The simulated cloud radiative effect changes by −1.43 W m −2 (6 %) and aerosol indirect radiative forcing over the industrial period changes by −0.10 W m −2 (10 %).

Ghosh, Pratapaditya [Carnegie Mellon University, P↗

DOE OSTI2023

Evaluation of Four Ground-based Retrievals of Cloud Droplet Number Concentration in Marine Stratocumulus with Aircraft In Situ Measurements

Cloud droplet number concentration (N d ) is crucial for understanding aerosol-cloud interactions (ACI) and associated radiative effects. We present evaluations of four ground-based N d retrievals based on comprehensive datasets from the Atmospheric Radiation Measurements (ARM) Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) field campaign. The N d retrieval methods use ARM ENA observatory ground-based remote sensing observations from a Micropulse lidar, Raman lidar, cloud radar, and the ARM NDROP Value-added Product (VAP), all of which also retrieve cloud effective radius (r e ). The retrievals are compared against aircraft measurements from the Fast-Cloud Droplet Probe (FCDP) and the Cloud and Aerosol Spectrometer (CAS) obtained from low-level marine boundary layer clouds on 12 flight days during summer and winter seasons. Additionally, the in situ measurements are used to validate the assumptions and characterizations used in the retrieval algorithms. Statistical comparisons of the probability distribution function (PDF) of the N d and cloud r e retrievals with aircraft measurements demonstrate that these retrievals align well with in situ measurements for overcast clouds, but they may substantially differ for broken clouds or clouds with low liquid water path (LWP). The retrievals are applied to four years of ground-based remote sensing measurements of overcast marine boundary layer clouds at the ARM ENA observatory to find that N d (r e ) values exhibit seasonal variations, with higher (lower) values during the summer season and lower (higher) values during the winter season. The ensemble of various retrievals using different measurements and retrieval algorithms such as those in this paper can help to quantify N d retrieval uncertainties and identify reliable N d retrieval scenarios. Of the retrieval methods, we recommend using the using the Micropulse lidar-based method given its good agreement with in situ measurements, it has less sensitivity to issues arising from precipitation and low cloud LWP/optical depth, and it has broad applicability by functioning for both day and nighttime conditions.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

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

One of the main goals of the Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Tracking Aerosol Convection Interactions Experiment (TRACER) field campaign near Houston, TX was to improve understanding of meteorology and aerosol effects on deep convective storms. To help TRACER achieve its goals of disentangling aerosol-cloud interactions from meteorology, the Texas A&M University (TAMU) team deployed the new fully mobile Rapid Onsite Atmospheric Measurement Van (ROAM-V) carrying instruments to measure aerosol and atmospheric properties that was moved to multiple locations on a deployment day of isolated convection initiated by the sea breeze.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

The Interaction Between Climate Forcing and Feedbacks

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

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

SAIL-Net Raw and Post Corrected POPS Data Fall 2021 - Summer 2023

SAIL-Net is a DOE funded project in the East River Watershed near Crested Butte, Colorado with the goal of advancing our understanding of aerosol-cloud interactions in complex, mountainous regions. Through the deployment of a network of six low cost microphysics nodes in Fall 2021 in the same domain at the SAIL campaign, SAIL-Net provides data on aerosol size distributions, cloud condensation nuclei (CCN), and ice nucleation particles (INP). This network enables the investigation of small-scale variations in complex terrain. Two datasets are provided - one containing raw data and the other containing post-corrected data. The raw dataset provides the raw data recorded from the POPS which were deployed at each of the six sites. These data are organized by site and broken down into daily data files. The six site names used here are: “gothic”, “irwin”, “cbtop”, “cbmid”, “pumphouse”, and “snodgrass”. These data are not cleaned or post-corrected, but some flags have been added. The data are reported at 1 second time resolution. The post-corrected dataset provides the post-corrected and cleaned data recorded from the POPS which were deployed at each of the six sites. This data are also organized by site (same as those found in the raw data) and broken down into daily data files. Unlike the raw POPS data, these data have already been cleaned to remove what we believe are bad values. These data should be ready to use with no cleaning. For a full description of the cleaning and post-correction process, see the readme.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

SAIL-Net CloudPuck CCN Data

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Earth System Model Aerosol–Cloud Diagnostics (ESMAC Diags) package, version 1: assessing E3SM aerosol predictions using aircraft, ship, and surface measurements

Abstract. An Earth system model (ESM) aerosol–cloud diagnostics package is developed to facilitate the routine evaluation of aerosols, clouds, and aerosol–cloud interactions simulated by the Energy Exascale Earth System Model (E3SM) from the US Department of Energy (DOE). The first version focuses on comparing simulated aerosol properties with aircraft, ship, and surface measurements, which are mostly measured in situ. The diagnostics currently cover six field campaigns in four geographical regions: eastern North Atlantic (ENA), central US (CUS), northeastern Pacific (NEP), and Southern Ocean (SO). These regions produce frequent liquid- or mixed-phase clouds, with extensive measurements available from the Atmospheric Radiation Measurement (ARM) program and other agencies. Various types of diagnostics and metrics are performed for aerosol number, size distribution, chemical composition, cloud condensation nuclei (CCN) concentration, and various meteorological quantities to assess how well E3SM represents observed aerosol properties across spatial scales. Overall, E3SM qualitatively reproduces the observed aerosol number concentration, size distribution, and chemical composition reasonably well, but it overestimates Aitken-mode aerosols and underestimates accumulation-mode aerosols over the CUS and ENA regions, suggesting that processes related to particle growth or coagulation might be too weak in the model. The current version of E3SM struggles to reproduce the new particle formation events frequently observed over both the CUS and ENA regions, indicating missing processes in current parameterizations. The diagnostics package is coded and organized in a way that can be extended to other field campaign datasets and adapted to higher-resolution model simulations.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Effective radiative forcing of anthropogenic aerosols in E3SM version 1: historical changes, causality, decomposition, and parameterization sensitivities

Abstract. The effective radiative forcing of anthropogenic aerosols (ERFaer) is an important measure of the anthropogenic aerosol effects simulated by a global climate model. Here we analyze ERFaer simulated by the E3SM version 1 (E3SMv1) atmospheric model using both century-long free-running atmosphere–land simulations and short nudged simulations. We relate the simulated ERFaer to characteristics of the aerosol composition and optical properties, and we evaluate the relationships between key aerosol and cloud properties. In terms of historical changes from the year 1870 to 2014, our results show that the global mean anthropogenic aerosol burden and optical depth increase during the simulation period as expected, but the regional averages show large differences in the temporal evolution. The largest regional differences are found in the emission-induced evolution of the burden and optical depth of the sulfate aerosol: a strong decreasing trend is seen in the Northern Hemisphere high-latitude region after around 1970, while a continued increase is simulated in the tropics. The relationships between key aerosol and cloud properties (relative changes between pre-industrial and present-day conditions) also show evident changes after 1970, diverging from the linear relationships exhibited for the period of 1870–1969. In addition to the regional differences in the simulated relationships, a reduced sensitivity in cloud droplet number and other cloud properties to aerosol perturbations is seen when the aerosol perturbation is large. Consequently, the global annual mean ERFaer magnitude does not increase after around 1970. The ERFaer in E3SMv1 is relatively large compared to the recently published multi-model estimates; the primary reason is the large indirect aerosol effect (i.e., through aerosol–cloud interactions). Compared to other models, E3SMv1 features large relative changes in the cloud droplet effective radius in response to aerosol perturbations. Large sensitivity is also seen in the liquid cloud optical depth, which is determined by changes in both the effective radius and liquid water path. Aerosol-induced changes in liquid and ice cloud properties in E3SMv1 are found to have a strong correlation, as the evolution of anthropogenic sulfate aerosols affects both the liquid cloud formation and the homogeneous ice nucleation in cirrus clouds (that causes a large effect on longwave ERFaer). As suggested by a previous study, the large ERFaer appears to be one of the reasons why the model cannot reproduce the observed global mean temperature evolution in the second half of the 20th century. Sensitivity simulations are performed to understand which parameterization and/or parameter changes have a large impact on the simulated ERFaer. The ERFaer estimates in E3SMv1 for the shortwave and longwave components are sensitive to the parameterization changes in both liquid and ice cloud processes. When the parameterization of ice cloud processes is modified, the top-of-model forcing changes in the shortwave and longwave components largely offset each other, so the net effect is negligible. This suggests that, to reduce the magnitude of the net ERFaer, it would be more effective to reduce the anthropogenic aerosol effect through liquid or mixed-phase clouds.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Freezing Processes in Southern Ocean Mixed Phase Clouds (Final Technical Report)

Southern Ocean (SO) low-level clouds remain a challenge for Earth system models to represent accurately. This project utilized DOE ARM observations and the Community Atmosphere Model (CAM) to improve process-level understanding of aerosol-cloud interactions and cloud microphysics for SO mixed-phase clouds. Specifically, our efforts include two main topics: 1) investigate the SO aerosol, cloud condensation nuclei (CCN), and ice nucleating particle (INP) population based on observations and determine predictive skill of simulating SO INPs, and 2) assess the ice formation pathways, including ice nucleation and secondary ice production, in SO mixed phase clouds utilizing a combination of observations and modeling tools. Studies focused on SO aerosol and INP resulted four manuscripts. Ice formation pathways in SO mixed phase clouds were investigated, revealing observed evidence of SIP active across all mixed phase temperatures. However, a key finding of this project is that despite significant progress in predicting SO INPs, the role of INP variability in SO cloud phase, precipitation, and radiative properties remain unknown due to challenges in microphysics parameterizations.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Characteristics and effects of aerosols during blowing snow events in the central Arctic

Sea salt aerosol (SSaer) significantly impacts aerosol-radiation and aerosol-cloud interactions, and sublimated blowing snow is hypothesized to be an important SSaer source in polar regions. Understanding blowing snow and other wind-sourced aerosols’ climate relevant properties is needed, especially during winter when Arctic amplification is greatest. However, most of our understanding of blowing snow SSaer comes from modeling studies, and direct observations are sparse. Additionally, SSaer can originate from multiple sources, making it difficult to disentangle emission processes. Here, we present comprehensive observations of wind-sourced aerosol during blowing snow events from the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition in the central Arctic. High wind speed strongly enhances total aerosol number, submicron sodium chloride mass, cloud condensation nuclei concentrations, and scattering coefficients. Generally, the relative response of aerosol properties to wind speed enhancement is strongest in fall when Arctic aerosol concentrations are lowest. Blowing snow events showed similar aerosol and environmental properties across events, apart from occasions with high snow age (>6 days since last snowfall). Coarse-mode number concentrations (>1 μm) are better explained by variability in wind speed averaged over 12-h air mass back trajectories arriving at the MOSAiC site compared to local, instantaneous wind speed, suggesting the importance of regional transport and consideration of air mass history for wind-driven aerosol production. These MOSAiC observations provide new insights into wind-driven aerosol in the central Arctic and may help validate modeling studies and improve model parameterizations particularly for aerosol direct and indirect radiative forcing.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2026

Atmospheric Composition and Radiative Forcing Effects due to UN International Ship Emissions Regulations (ACRUISE) Field Campaign Report

Aerosols, or atmospheric particulates, are long known to be able to seed clouds and modify their characteristics (e.g., cloud brightness, coverage, lifetime). However, the impact of aerosols on clouds is highly complex and non-linear. As a result, aerosol-cloud interaction remains the largest uncertainty in our understanding of the Earth’s radiative balance and in any future climate projections. Aerosols are also a principal component of air pollution and are known to adversely affect respiratory and cardiovascular health.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

General circulation models simulate negative liquid water path–droplet number correlations, but anthropogenic aerosols still increase simulated liquid water path

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.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Opinion: A critical evaluation of the evidence for aerosol invigoration of deep convection

Deep convective updraft invigoration via indirect effects of increased aerosol number concentration on cloud microphysics is frequently cited as a driver of correlations between aerosol and deep convection properties. Here, we critically evaluate the theoretical, modeling, and observational evidence for warm- and cold-phase invigoration pathways. Though warm-phase invigoration is plausible and theoretically supported via lowering of the supersaturation with increased cloud droplet concentration in polluted conditions, the significance of this effect depends on substantial supersaturation changes in real-world convective clouds that have not been observed. Much of the theoretical support for cold-phase invigoration depends on unrealistic assumptions of instantaneous freezing and unloading of condensate in growing, isolated updrafts. When applying more realistic assumptions, impacts on buoyancy from enhanced latent heating via fusion in polluted conditions are largely canceled by greater condensate loading. Many foundational observational studies supporting invigoration have several fundamental methodological flaws that render their findings incorrect or highly questionable. Thus, much of the evidence for invigoration has come from numerical modeling, but different models and setups have produced a vast range of results. Furthermore, modeled aerosol impacts on deep convection are rarely tested for robustness, and microphysical biases relative to observations persist, rendering many results unreliable for application to the real world. Without clear theoretical, modeling, or observational support, and given that enervation rather than invigoration may occur for some deep convective regimes and environments, it is entirely possible that the overall impact of cold-phase invigoration is negligible. Substantial mesoscale variability of dominant thermodynamic controls on convective updraft strength coupled with substantial updraft and aerosol variability in any given event are poorly quantified by observations and present further challenges to isolating aerosol effects. Observational isolation and quantification of convective invigoration by aerosols is also complicated by limitations of available cloud condensation nuclei and updraft speed proxies, aerosol correlations with meteorological conditions, and cloud impacts on aerosols. Furthermore, many cloud processes, such as entrainment and condensate fallout, modulate updraft strength and aerosol–cloud interactions, varying with cloud life cycle and organization, but these processes remain poorly characterized. Considering these challenges, recommendations for future observational and modeling research related to aerosol invigoration of deep convection are provided.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Opportunistic experiments to constrain aerosol effective radiative forcing

Aerosol–cloud interactions (ACIs) are considered to be the most uncertain driver of present-day radiative forcing due to human activities. The nonlinearity of cloud-state changes to aerosol perturbations make it challenging to attribute causality in observed relationships of aerosol radiative forcing. Using correlations to infer causality can be challenging when meteorological variability also drives both aerosol and cloud changes independently. Natural and anthropogenic aerosol perturbations from well-defined sources provide “opportunistic experiments” (also known as natural experiments) to investigate ACI in cases where causality may be more confidently inferred. These perturbations cover a wide range of locations and spatiotemporal scales, including point sources such as volcanic eruptions or industrial sources, plumes from biomass burning or forest fires, and tracks from individual ships or shipping corridors. We review the different experimental conditions and conduct a synthesis of the available satellite datasets and field campaigns to place these opportunistic experiments on a common footing, facilitating new insights and a clearer understanding of key uncertainties in aerosol radiative forcing. Cloud albedo perturbations are strongly sensitive to background meteorological conditions. Strong liquid water path increases due to aerosol perturbations are largely ruled out by averaging across experiments. Opportunistic experiments have significantly improved process-level understanding of ACI, but it remains unclear how reliably the relationships found can be scaled to the global level, thus demonstrating a need for deeper investigation in order to improve assessments of aerosol radiative forcing and climate change.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗