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At least 37 records · Page 2

Impact of Turbulence Representation on the Relationship Between Cloud Feedback and Aerosol‐Cloud Interaction in an E3SMv2 Perturbed Parameter Ensemble

Recent studies reveal an anti‐correlation between global cloud feedback (CF) and effective radiative forcing due to aerosol‐cloud interaction (ERFaci) in Earth system models, but the physical mechanisms underlying it remain uncertain. Here we investigate how different turbulence representations contribute to this relationship over the global ocean using an ensemble of Energy Exascale Earth System Model version 2 simulations with perturbed turbulence parameters. The anti‐correlation appears only in the tropical ascent regime. In the Northern Hemisphere midlatitude and high latitude regimes, there is no significant correlation, and in the tropical marine low cloud and Southern Ocean regimes, the correlation is positive. These opposite correlations are primarily driven by opposing CF responses to perturbed parameters. We find that the mean‐state turbulent mixing strength affects both CF and ERFaci, enabling strong correlations in certain regimes. This study highlights the complex linkages between CF and ERFaci through turbulent processes across diverse cloud regimes.

54 ENVIRONMENTAL SCIENCES

Interconnection of Aerosol‐Cloud Interactions and Cloud Feedback Through Warm Rain Process

Recent research has revealed a correlation within the Coupled Model Intercomparison Project Phase 6 (CMIP6) simulations: models exhibiting more pronounced warming due to positive cloud feedback simultaneously show enhanced cooling from aerosol‐cloud interactions (ACI). However, the interplay between ACI and cloud feedback is not well understood in these models. Our study addresses this gap by modifying the autoconversion rate in two Earth system models (ESMs), elucidating how ACI could connect with cloud feedback through the warm rain process. We find that higher autoconversion rates, which are associated with stronger ACI, suppress the increase in cloud liquid water path (LWP) and cloud optical depth with warming by enhancing the precipitation efficiency over the extratropical regions, leading to a larger positive cloud feedback. This study offers new insights into the compensatory mechanism between ACI and cloud feedback through the warm rain process and highlights the importance of constraining the autoconversion parameterization in models.

54 ENVIRONMENTAL SCIENCES

Synthesis of aerosol-cloud interactions over the southeast Atlantic throughout the seasonal cycle (Final Technical Report)

An analysis of the aerosol compositional, physical and optical datasets towards understanding why the single‐scattering‐albedo of smoke is so much lower over the southeast Atlantic than elsewhere, in particular the northern hemisphere. This includes data from the complementary NASA ORACLES aircraft campaign, which sampled closer to the African coast. The first analysis resulting from this prong of research was published earlier this year (Dobracki et al., 2023, ACP) and focused more on the free-tropospheric biomass burning aerosol (BBA). We primarily attributed the low SSA to a high number/mass fraction of black carbon, ranging from 15 to 40% of the total aerosol. We are further able to use other literature, the modified combustion efficiency, and the black carbon and carbon monoxide values to highlight a common source in dry, flame-efficient burning conditions of grasses. Condensation and coagulation of smaller aerosol particles onto the larger black carbon aerosols can also increased the SSA as the aerosol ages from 4 to 5 days. A comparison to data gathered over Ascension Island during the UK CLARIFY aircraft campaign indicates an organic aerosol loss relative to black carbon of about 50%. This is high compared to findings from other campaigns.

54 ENVIRONMENTAL SCIENCES

Quantifying the impacts of marine aerosols over the southeast Atlantic Ocean using a chemical transport model: implications for aerosol–cloud interactions

The southeast Atlantic region, characterized by persistent stratocumulus clouds, has one of the highest uncertainties in aerosol radiative forcing and significant variability across climate models. In this study, we analyze the seasonally varying role of marine aerosol sources and identify key uncertainties in aerosol composition at cloud-relevant altitudes over the southeast Atlantic using the GEOS-Chem chemical transport model. We evaluate simulated aerosol optical depth (AOD) and speciated aerosol concentrations against those collected from ground observations and aircraft campaigns such as LASIC, ORACLES, and CLARIFY, conducted during 2017. The model consistently underestimates AOD relative to AERONET, particularly at remote locations like Ascension Island. However, when compared with aerosol mass concentrations from aircraft campaigns during the biomass burning period, it performs adequately at cloud-relevant altitudes, with a normalized mean bias (NMB) between -3.5 % (CLARIFY) and -7.5 % (ORACLES). At these altitudes, in the model, organic aerosols (63 %) dominate during the biomass burning period, while sulfate (41 %) prevails during austral summer, when dimethylsulfide (DMS) emissions peak in the model. Our findings indicate that marine sulfate can account for up to 69 % of total sulfate during the high-DMS period. Sensitivity analyses indicate that refining DMS emissions and oxidation chemistry may increase sulfate aerosol produced from marine sources, highlighting that there remains large uncertainty as to the role of DMS emissions in the marine boundary layer. Additionally, we find marine primary organic aerosol emissions may substantially increase total organic aerosol concentrations, particularly during austral summer. This study underscores the imperative need to refine marine emissions and their chemical transformations, as aerosols from marine sources are a major component of total aerosols at cloud-relevant altitudes and may impact uncertainties in aerosol radiative forcing over the southeast Atlantic.

54 ENVIRONMENTAL SCIENCES

A Concept of a Convection–Cloud Chamber to Study Aerosol–Cloud–Drizzle Interactions

Understanding and quantifying the full chain of processes from aerosol activation to drizzle formation, and the associated feedbacks to the aerosol chemical and physical properties, all within a turbulent cloud are some of the toughest challenges in atmospheric chemistry and physics and are keys to the cloud–precipitation puzzle. This paper describes a concept for a new type of research facility consisting of a cloud chamber plus associated instrumentation and computational models, to explore aerosol–cloud interactions and processing, cloud optical properties, entrainment–cloud interactions, and quantitative assessment of drizzle onset. The envisioned design is for a 3 m × 3 m × 9 m chamber, such that the height is sufficient to achieve long lifetimes for aerosol processing and for significant drizzle growth by collision and coalescence. A suite of computational tools for simulating microphysical properties in the chamber provides a digital twin for designing the chamber and a range of example experiments. Theory and test results from novel remote sensing systems for exploring chemical and physical interactions and evolution of aerosols, cloud droplets, and drizzle within turbulent clouds are described. Testing of technology needed for the operation of a large-volume chamber, including aerosol generation methods and novel materials for water vapor boundary conditions, is described. Simulations suggest that spatially uniform turbulence and microphysical properties can be sustained in a steady state, with reasonable aerosol and water vapor fluxes, and that substantial drizzle can be produced through collision and coalescence of cloud droplets. Remaining challenges for more detailed engineering design and a discussion of possible first-light experiments are described.

54 ENVIRONMENTAL SCIENCES

Improving the Confidence in Retrievals of Vertical Distributions of Cloud Condensation Nuclei Number Concentration from ARM Supported by Aircraft In Situ Observations

Accurate quantification of the vertical distribution of cloud condensation nuclei (CCN) number concentrations is critical for improving our understanding of aerosol–cloud interactions. Ground-based Raman lidars operated by the Atmospheric Radiation Measurement (ARM) program, together with surface CCN measurements, are used to retrieve vertically resolved CCN number concentrations (Retrieved Number concentration of CCN, RNCCN). These retrievals rely on several assumptions, including that aerosol composition is vertically homogeneous. To assess this assumption, we developed and tested a framework to infer the dominant aerosol classes/types at different altitudes. This was done by applying a k-Nearest-Neighbors (kNN) algorithm to lidar ratio and linear depolarization ratio measurements from Raman lidar. We evaluated the framework using aircraft aerosol and CCN measurements from the ARM Holistic Interactions of Shallow Clouds, Aerosols, and Land Ecosystems (HI-SCALE) field campaign. The results show that RNCCN performance degrades as vertical aerosol complexity increases, i.e., RNCCN agrees with the aircraft CCN in vertically homogeneous conditions, but closure decreases in layered aerosol structures. To generalize beyond individual examples, we introduce a metric (heterogeneity index) that quantifies the vertical complexity by assessing the variation of inferred aerosol classes/types. Case-level statistics show a tendency for RNCCN and aircraft differences to increase with this metric. By detecting retrievals that are likely compromised by aerosol vertical heterogeneity, the proposed framework improves the interpretability and effective use of RNCCN used for long-term evaluation of models and aerosol–cloud interactions.

Tian, Jingjing

Competition response of cloud supersaturation explains diminished Twomey effect for smoky aerosol in the tropical Atlantic

The Twomey effect brightens clouds by increasing aerosol concentrations, which activates more droplets and decreases cloud supersaturation in response to more competition for water vapor. To quantify this competition response, we used marine low cloud observations in clean and smoky conditions at Ascension Island in the tropical South Atlantic during the Layered Aerosol Smoke Interactions with Cloud (LASIC) campaign. These observations show similar increases in droplet number for increased accumulation-mode particles from surface-based and satellite cloud retrievals, demonstrating the importance of below-cloud aerosol measurements for retrieving aerosol–cloud interactions (ACI) in clean and smoky aerosol conditions. Four methods for estimating cloud supersaturation from aerosol–cloud measurements were compared, with cloud scene-based and parcel-based methods showing sufficient variability for a strong dependence on both aerosol accumulation number concentration and cloud-base updraft velocities. Decomposing aerosol-related changes in cloud albedo and optical depth shows the calculated competition response accounts for dampening the activation response by 12 to 35%, explaining the diminished Twomey effect at high aerosol concentrations observed for smoky conditions at LASIC and previously around the world. This result was consistent for independent supersaturation retrievals by cloud scene-based droplet number and cloud condensation nuclei and parcel-based multimode size-resolving Lagrangian methods. Translating aerosol effects to local radiative forcing with clean conditions as a proxy for preindustrial and smoky conditions for present-day showed that the competition response reduces cooling from the Twomey radiative forcing by 12 to 35%, providing an essential process-specific constraint for improving the representation of aerosol competition in climate model simulation of indirect aerosol forcing.

54 ENVIRONMENTAL SCIENCES

Large spatiotemporal variability in aerosol properties over central Argentina during the CACTI field campaign

Abstract. Few field campaigns with extensive aerosol measurements have been conducted over continental areas in the Southern Hemisphere. To address this data gap and better understand the interactions of convective clouds and the surrounding environment, extensive in situ and remote sensing measurements were collected during the Cloud, Aerosol, and Complex Terrain Interactions (CACTI) field campaign conducted between October 2018 and April 2019 over the Sierras de Córdoba range of central Argentina. This study describes measurements of aerosol number, size, composition, mixing state, and cloud condensation nuclei (CCN) collected on the ground and from a research aircraft during 7 weeks of the campaign. Large spatial and multiday variations in aerosol number, size, composition, and CCN were observed due to transport from upwind sources controlled by mesoscale to synoptic-scale meteorological conditions. Large vertical wind shears, back trajectories, single-particle measurements, and chemical transport model predictions indicate that different types of emissions and source regions, including biogenic emissions and biomass burning from the Amazon and anthropogenic emissions from Chile and eastern Argentina, contribute to aerosols observed during CACTI. Repeated aircraft measurements near the boundary layer top reveal strong spatial and temporal variations in CCN and demonstrate that understanding the complex co-variability of aerosol properties and clouds is critical to quantify the impact of aerosol–cloud interactions. In addition to quantifying aerosol properties in this data-sparse region, these measurements will be valuable to evaluate predictions over the midlatitudes of South America and improve parameterized aerosol processes in local, regional, and global models.

54 ENVIRONMENTAL SCIENCES

Investigating Aerosol Hygroscopicity in the Subcloud Transition Zone and at the Surface in the Southern Great Plains

Aerosols beneath a cloud base, a subcloud transition zone (SCTZ), are key to understand both the aerosol-cloud interaction and aerosol-radiation interactions. Lidars have been the primary means of observing aerosols in the SCTZ by virtue of enhanced light scattered by aerosol particles. The enhanced light maybe caused by several factors: the aerosol swelling effect due to hygroscopicity under high relative humidity, cloud 3-dimensional (3D) effect, aerosol nucleation into cloud droplets, etc. While each factor and process has been known, their relative contributions are much poorly quantified. This study explores the hygroscopicity and optical properties of aerosols in the SCTZ and at ground level in the Southern Great Plains (SGP) region. Utilizing comprehensive observational data from the U.S. Department of Energy's Atmospheric Radiation Measurement at the Oklahoma SGP site, including ground-based aerosol measurements and Raman lidar profiles from April 2021 to April 2022, this study extensively analyzes the influence of aerosol hygroscopic growth and cloud fragments on aerosol optical properties. Distinct seasonal variations in aerosol hygroscopic characteristics are revealed. At the ground level, aerosols in autumn and winter exhibit stronger hygroscopicity due to a higher proportion of inorganic content than summer. In the SCTZ, aerosols during summer show enhanced backscatter due to strong cloud fragmentation effects, with numerous cloud fragments elevating hygroscopicity beyond that observed in autumn and winter. These insights are crucial for understanding the interactions between aerosols at the surface and cloud layers, evaluating cloud condensation nuclei beneath clouds, and their implications for atmospheric radiation and climate modeling.

Hu, Rong [Beijing Normal University, Beijing (Chin

Strategizing emission cuts in China to mitigate short-term warming from clean air policies

Aerosol-cloud interactions remain one of the largest sources of uncertainty in estimates of anthropogenic climate forcing. Reducing aerosols to achieve air quality improvement and climate goals can cause unintended warming due to the weakening of aerosol cooling. Here we investigate the climate impacts of spatially optimized sulfur dioxide (SO 2 ) emission reduction under a carbon-neutral pathway in China. We find that targeting reduction in highly polluted regions in China significantly suppresses the rise in effective radiative forcing due to aerosol-cloud interactions (ERF aci ) during 2020–2060. Owing to the nonlinear aerosol-cloud interaction, the optimized emission reduction strategy limits the regional average increase in ERF aci of more than 0.89 W m −2 to less than 0.13 W m −2 in the short-term future during 2020–2040 and weakens the ERF aci increase by two-thirds in 2060 over China. These findings demonstrate the critical role of targeted emission control in mitigating short-term climate risks while pursuing air quality goals.

Zhu, Yitong [Nanjing Univ. of Information Science

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

Enhanced mid-latitude warming due to poleward shift of sea salt aerosols in a warmer future

Natural aerosols provide large uncertainties regarding the quantification of the climate effects of aerosols, especially those related to aerosol-cloud interactions. Advancing research on the interaction of natural aerosols and climate can provide a better assessment of the climate impacts of anthropogenic activities. Furthermore, as one of the most dominant natural aerosols, sea salt has the highest proportion of mass in natural aerosols. Sea salt can be regarded as a purely scattering aerosol, causing a negative radiative effect by scattering shortwave solar radiation and acting as cloud condensation nuclei (CCN) through aerosol-cloud interactions. Future climate change will influence sea salt distribution, thus modifying the radiative effects of sea salt, which will further affect the climate. However, few previous studies have explored the interactions between sea salt changes under warming scenarios and climate change.

Yang, Yang [Nanjing Univ. of Information Science a

Characterization of Organosulfates and Organonitrates in Vertically Resolved Aerosols over the Southern Great Plains Field Campaign Report

Aerosol is the largest individual source of uncertainty in assessing the Earth’s radiative balance due to poorly understood aerosol processes and aerosol-cloud interactions. Thus, to constrain aerosol’s climate impacts, it is critical to understand aerosol compositions at high elevations. Organic material accounts for about 20-80% of total aerosol mass in the atmosphere and is known to play a key role in aerosol processes and cloud formation. In prior research, characterization of aerosol molecular composition has been mostly carried out at ground level. In these ground-level measurements, total speciated organosulfates and organonitrates may contribute significantly to organic aerosol mass on the order of 10-40%, most of which are from abundant biogenic volatile organic compounds such as isoprene and monoterpenes. Organosulfates and organonitrates have also been shown to be present in substantial amounts in cloud water, suggesting that they can be transported and/or directly formed at high elevations. On the other hand, the less common and more expensive aircraft studies have performed high-altitude measurements, but were often limited in the number of different altitudes sampled and in sample collection under consistent conditions. Therefore, the vertical distributions of key aerosol components such as organosulfates and organonitrates are not well understood and have not been extensively studied. Nevertheless, it is important to understand how organosulfates and organonitrates in aerosols are distributed, transformed, participate in aqueous-phase processes, and interact with high-altitude clouds.

54 ENVIRONMENTAL SCIENCES

Boundary Layer Exploration of Aerosols and Clouds ON Ships (BEACONS)

BEACONS aims to demonstrate autonomous deployment of a shipborne system that routinely observes atmospheric, cloud, and aerosol properties. These observations enable scientists to study aerosol-cloud interactions, advancing energy resilience and the Department of Energy's mission to improve model prediction. Key Project Outcomes Autonomous deployment of aerosol and cloud measurement systems aboard a Pasha Hawaii Marjorie C commercial ship. Six-month campaign for continuous, high-resolution aerosol and cloud data collection with minimal crew intervention. Development and testing of instruments in two phases, advancing from essential to complex systems. AI-ready processed data on the BEACONS Data Platform for near-real-time data access. Validation of aerosol-cloud interaction hypotheses for improved modeling. Establishment of best practices for instrument deployment in marine environments. Scientific collaboration to support the U.S. Department of Energy (DOE) Biological and Environmental Research (BER) mission.

54 ENVIRONMENTAL SCIENCES

Investigating Spatial Variability of Aerosol, Cloud Condensation Nuclei, and Ice Nucleating Particles in Mountainous Terrain Field Campaign Report

The U.S. Department of Energy Atmospheric System Research (ASR)-supported Surface Atmosphere Integrated Field Laboratory (SAIL) campaign in the East River Watershed (ERW) of the Upper Colorado River Basin in southwestern Colorado ran from fall 2021 to spring 2023. Two monitoring sites were deployed in the ERW as part of SAIL. The two sites were the Aerosol Observation System (AOS) located on Crested Butte Ski Mountain, and the second ARM Mobile Facility (AMF2), located at the Rocky Mountain Biological Laboratory in Gothic, Colorado. To gain a more comprehensive understanding of aerosols in complex, mountainous terrain, Handix Scientific deployed SAIL-Net, a distributed network of six measurement nodes spanning the domain of the SAIL research area from October 2021 to July 2023. Each node measured aerosol particles between 140 nm and 3.4 μm in diameter using a small portable optical particle spectrometer (POPS; Gao et al. 2016), cloud condensation nuclei (CNN) using a miniature CCN counter (CloudPuck), and ice nucleating particles (INP) using the time-resolved aerosol filter sampler (TRAPS; Creamean et al. 2018). Our approach was similar to other studies that aimed to better characterize and understand aerosols and gas-phase pollutants using networks of lower-cost sensors (Caubel et al. 2019, Kelly et al. 2021, Asher et al. 2022). Such studies have identified neighborhood-level variations in pollutant concentrations (Schneider et al. 2017, Popoola et al. 2018, Caubel et al. 2019). Small-scale variations such as this are poorly represented in models and poorly measured by a single monitoring system (Caubel et al. 2019). Previous work has shown the representation error (the ability of measurements to represent a larger area) increases with complex orography, leading to decreases in model accuracy (Schutgens et al. 2017). The overall goal of SAIL-Net was to improve our understanding of the variability of aerosol in the ERW, thus increasing our knowledge of aerosol-cloud interactions in this region and informing the usefulness of distributed networks of measurements for future studies. We met this goal by answering the following science questions: 1. What is the aerosol temporal variability, and how does aerosol inhomogeneity vary seasonally? Is there significant seasonal variability in sources, or are short-term meteorological conditions the most important determining factor in sources for cloud nuclei? 2. What is the aerosol spatial variability? What are the aerosol characteristics at cloud base, presumably the particles most representative of those acting as cloud nuclei? 3. How should measurement networks be designed to capture aerosol-cloud interactions, and what do they need to measure? Can a single measurement site accurately represent aerosol properties in regions of complex terrain? SAIL-Net consisted of six measurement nodes spread across the ERW near Crested Butte, Colorado. The primary objective in site placement was to select locations that captured the vertical variation in aerosol properties while also spanning the domain of the SAIL campaign. The elevation of the sites ranged from roughly 2750 m along the valley floor of the ERW to approximately 3500 m near the top of Crested Butte Mountain, which is one of the taller peaks in the ERW. The farthest distance between sites was 14 km, while the closest two sites were approximately 1 km apart. Two of the sites were collocated with the ARM SAIL sites; our instruments sat on top of one of the trailers at AOS and another one of our sites was located in a meadow just above AMF2.

54 ENVIRONMENTAL SCIENCES

Sensitivity of Anthropogenic Cloud Droplet Number Change to Preindustrial Emission Inventories and Physics Parameterizations

Understanding the preindustrial (PI) to present-day (PD) change in cloud droplet number concentration (ΔNd) is important to constrain the anthropogenic influence on clouds and aid future model projections. Perturbed parameter ensemble simulations of PI and PD conditions in the Energy Exascale Earth System Model (E3SMv3) reveal two locations with consistent negative ΔNd signal across parameter space–the Southeastern US and the United Kingdom–despite a trend of positive ΔNd globally from increased fossil fuel consumption. These negative ΔNd signals are driven by higher anthropogenic biofuel emissions in the PI. By varying the PI aerosol mass and/or number emissions across these data sets' uncertainty ranges, we can change the magnitude and sign of ΔNd and the effective radiative forcing from aerosol-cloud interactions (ERFaci) regionally and globally, with near-zero ΔNd leading to near-zero ERFaci. These results highlight the need to constrain PI emission uncertainty to better understand Earth system responses to aerosol-cloud interactions.

Brown, Hunter Y. [University of Wyoming, Laramie,