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At least 1,747 records · Page 97

Uncertainty in Aerosol–Cloud Radiative Forcing Is Driven By Clean Conditions

Atmospheric aerosols and their impact on cloud properties remain the largest uncertainty in the human forcing of the climate system. By increasing the concentration of cloud droplets (Nd), aerosols reduce droplet size and increase the reflectivity of clouds (a negative radiative forcing). Central to this climate impact is the susceptibility of cloud droplet number to aerosol (β), the diversity of which explains much of the variation in the radiative forcing from aerosol–cloud interactions (RFaci) in global climate models. This has made measuring β a key target for developing observational constraints of the aerosol forcing.

Edward Gryspeerdt↗

Satellite Tracking of Shallow Cumulus during CAMP2Ex: The Aerosol and Organization Connection

Shallow moist convection is ubiquitous throughout the tropics and represents a key player in boundary layer processes. Shallow clouds come in many forms, from scattered, short-lived cumulus to organized features that include cold pool boundaries and lines reaching O(100 km) scale lasting several hours. In this study, we explore how cloud morphology and environmental aerosol affect shallow cumulus lifecycle properties. Measuring such influences requires a broad, detailed view of these cloud fields as they grow and decay. Geostationary satellites provide a means to follow the clouds with enhanced spatiotemporal sampling from space. We apply a cloud-tracking tool to study lifecycle properties of shallow cumulus sampled during the NASA Cloud, Aerosol, and Monsoon Processes Philippines Experiment (CAMP2Ex) field campaign of 2019. The mission conducted airborne and shipborne operations over the West Pacific Ocean, in tandem with Rapid Scan imagery from the Advanced Himawari Imager (AHI) on the Japan Meteorological Agency’s (JMA) Himawari-8 satellite. We segment shallow cumulus on AHI 0.5-km visible reflectance during the daylit hours of several research flights that exhibited ideal atmospheric conditions for tracking. We collect the resulting cloud tracks by regions containing airborne sampling of the cloud environments and by two specific segmentation techniques: one optimized for small, disorganized cumulus and the other for larger, organized clouds using suitable thresholds for reflectance and blurring. We present an analysis of cloud lifecycle properties using our dual segmentation approach for various sampled environments of CAMP2Ex. A total of 7 research flights (RFs) exhibited ideal conditions for generating cloud-track ensembles under similar thermodynamic and kinematic profiles but with varying aerosol load. We consider lifetime, track-achieved metrics, and ensemble-fitted growth rates to evaluate the aerosol effect. Cloud elongation, a factor in cloud morphology, is also considered for any potential influence in observed shifts in growth rates. The results suggest that aerosol affects cloud lifecycles more significantly for clouds with larger areas and independent of the elongation factor.

Cloud Tracking↗

Performance of Heterogeneous Sulfate Aerosol Formation Mechanisms Against Aircraft and Ground-Based Observations in Seoul, South Korea

Haze events are a common occurrence in East Asia, where local meteorology combines with anthropogenic emissions under certain conditions to create rapid increases in secondary aerosol. Often these events are driven by rapid production of secondary sulfate-nitrate-ammonium (SIA) aerosol. Models have typically included simple parameterizations of the production of sulfate during these events which vary widely in their magnitude. There are a range of different mechanistic descriptions of the chemical processes occurring during these events in large part due to poor constraints on aerosol pH and transition metal content, both of which are important to determining the key pathway(s) driving aerosol production. Here, we use the GEOS-Chem chemical transport model to interpret detailed ground and aircraft observations from May and June 2016 during the Korea-United States Air Quality (KORUS-AQ) field study to evaluate the mechanistic pathways governing sulfate production during a haze event. We apply our model of sulfate production mechanisms to ground-based speciated aerosol measurements in winter, summer, and fall in Seoul.

Katherine R Travis↗

Evaluation of Aerosol Data Assimilation and Forecasts in the NASA GEOS Model during the ASIA-AQ Campaign

Fine particulate matter (PM2.5) poses significant risks to human health and the environment by penetrating the lungs and causing respiratory and cardiovascular diseases, making it crucial to understand its sources and behavior for effective air quality management. The Goddard Earth Observing System (GEOS) Forward Processing (FP) system model, operated by the Global Modeling and Assimilation Office (GMAO) at NASA's Goddard Space Flight Center, provides real-time weather and aerosol analyses and forecasts. In addition to meteorological data assimilation, the GEOS-FP system also assimilates aerosol using Moderate Resolution Imaging Spectroradiometer (MODIS) Aerosol Optical Depth (AOD) and Aerosol Robotic Network (AERONET) AOD data. In this study, the aerosol data assimilation and forecasts performance of the GEOS-FP model were evaluated for predicting PM2.5 in Korea using observations from the Airborne and Satellite Investigation of Asian Air Quality (ASIA-AQ) campaign. The ASIA-AQ campaign, an international collaborative field study initiative, aims to enhance understanding of local air quality issues and address common challenges in interpreting satellite data and air quality modeling. Conducted in South Korea from February 15 to March 13, 2024, during the high PM2.5 concentration winter season, this campaign provided extensive airborne and ground observations for intensive analysis of PM2.5 model simulations. We demonstrate how the assimilation runs and the forecasting performance of PM2.5 at 24-hour and 48-hour intervals vary. Additionally, we analyzed the differences and characteristics of PM2.5 composition in cases of long-range transport and local emissions. Using ASIA-AQ airborne data, we also examined the vertical profile of fine particulate matter. Through the intensive observations of this campaign, the GEOS model was assessed over South Korea using both in situ and airborne measurements to establish a baseline and identify priorities for future development.

Seunghee Lee↗

Aerosol–Ice Formation Closure: A Southern Great Plains Field Campaign

Prediction of ice formation in clouds presents one of the grand challenges in the atmospheric sciences. Immersion freezing initiated by ice-nucleating particles (INPs) is the dominant pathway of primary ice crystal formation in mixed-phase clouds, where supercooled water droplets and ice crystals coexist, with important implications for the hydrological cycle and climate. However, derivation of INP number concentrations from an ambient aerosol population in cloud-resolving and climate models remains highly uncertain. We conducted an aerosol–ice formation closure pilot study using a field-observational approach to evaluate the predictive capability of immersion freezing INPs. The closure study relies on collocated measurements of the ambient size-resolved and single-particle composition and INP number concentrations. The acquired particle data serve as input in several immersion freezing parameterizations, which are employed in cloud-resolving and climate models, for prediction of INP number concentrations. We discuss in detail one closure case study in which a front passed through the measurement site, resulting in a change of ambient particle and INP populations. We achieved closure in some circumstances within uncertainties, but we emphasize the need for freezing parameterization of potentially missing INP types and evaluation of the choice of parameterization to be employed. Overall, this closure pilot study aims to assess the level of parameter details and measurement strategies needed to achieve aerosol–ice formation closure. Furthermore, the closure approach is designed to accurately guide immersion freezing schemes in models, and ultimately identify the leading causes for climate model bias in INP predictions.

58 GEOSCIENCES↗

Quantifying and Modeling the Impact of Phase State on the Ice Nucleation Abilities of 2-Methyltetrols as a Key Component of Secondary Organic Aerosol Derived from Isoprene Epoxydiols

Organic aerosols (OAs) may serve as ice-nucleating particles (INPs), impacting the formation and properties of cirrus clouds when their phase state and viscosity are in the semisolid to glassy range. However, there is a lack of direct parameterization between aerosol viscosity and their ice nucleation capabilities. In this study, we experimentally measured the ice nucleation rate of 2-methyltetrols (2-MT) aerosols, a key component of isoprene-epoxydiol-derived secondary organic aerosols (IEPOX-SOA), at different viscosities. These results demonstrate that the phase state has a significant impact on the ice nucleation abilities of OA under typical cirrus cloud conditions, with the ice nucleation rate increasing by 2 to 3 orders of magnitude when the phase state changes from liquid to semisolid. An innovative parametric model based on classical nucleation theory was developed to directly quantify the impact of viscosity on the heterogeneous nucleation rate. This model accurately represents our laboratory measurement and can be implemented into climate models due to its simple, equation-based form. Based on data collected from the ACRIDICON-CHUVA field campaign, our model predicts that the INP concentration from IEPOX-SOA can reach the magnitude of 1 to tens per liter in the cirrus cloud region impacted by the Amazon rainforest, consistent with recent field observations and estimations. This novel parameterization framework can also be applied in regional and global climate models to further improve representations of cirrus cloud formation and associated climate impacts.

2-methyltetrol↗

Effects of Sucrose on Phase Transitions of Organic/Inorganic Aerosols

Aerosol morphology influences the interactions of particles with light, water uptake, and heterogeneous chemistry. Through these mechanisms, morphology may be important to the role of aerosol particles on the climate system. A factor that impacts morphology is the diverse and complex mixture of organic compounds that make up the aerosol particles in the atmosphere. In this paper, we investigate the effect of sucrose on liquid-liquid phase separation. As the amount of sucrose is increased, the oxygen to carbon ratio (O:C) of the particles increases. We demonstrate that the morphology of the particle changes as O:C is increased with phase separation causing the particle to take on a textured appearance due to large or small inclusions, as opposed to a core-shell particle. As a result of the increased O:C ratio, the separation relative humidity (SRH) of the particles decreases and, in all cases, the SRH can be completely arrested with the addition of a sufficiently large concentration of sucrose. The quantity of sucrose required to arrest phase separation of the particles shows a direct correlation with the SRH of the system without sucrose. The identity of the salt further impacts the amount of sucrose required to arrest phase separation and is controlled more strongly by the identity of the anion. When the mixture contains an organic/inorganic combination that is strongly phase separating, phase separation is observed at an O:C of 0.92 which is a higher O:C value than previously shown (O:C > 0.8). Sucrose is compared with several other high O:C compounds to confirm the influence of the average O:C ratio. In all, these effects could drastically influence aerosol processes in the climate system.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Modeling the Size Distribution and Chemical Composition of Secondary Organic Aerosols during the Reactive Uptake of Isoprene-Derived Epoxydiols under Low-Humidity Condition

Reactive uptake of isoprene epoxydiols (IEPOX), which are isoprene oxidation products, onto acidic sulfate aerosols is recognized to be an important mechanism for the formation of isoprene-derived secondary organic aerosol (SOA). While a mechanistic understanding of IEPOX-SOA formation exists, several processes affecting their formation remain uncertain. Evaluating mechanistic IEPOX-SOA models with controlled laboratory experiments under longer atmospherically relevant timescales is critical. Here, we implement our latest understanding of IEPOX-SOA formation within a box model to simulate the measured reactive uptake of IEPOX on polydisperse ammonium bisulfate seed aerosols within an environmental Teflon chamber. The model is evaluated with single-particle measurements of size distribution, volume, density, and composition of aerosols due to IEPOX-SOA formation at timescales of hours. Additionally, we find that the model can simulate the growth of particles due to IEPOX multiphase chemistry, as reflected in increases of the mean particle size and volume concentrations, and a shift of number size distribution to larger sizes. The model also predicts the observed evolution of particle number mean diameter and total volume concentrations at the end of the experiment. We show that in addition to self-limiting effects of IEPOX-SOA coatings, accounting for the molar balance between inorganic and organic sulfate and mass accommodation coefficient of IEPOX are important parameters governing modeling of IEPOX-SOA formation. Thus, models which do not account for the molar sulfate balance and/or diffusion limitations within IEPOX-SOA coatings are likely to predict too high IEPOX-SOA formation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Observations of Fog-Aerosol Interactions Over Central Greenland

Supercooled fogs can have an important radiative impact at the surface of the Greenland Ice Sheet, but they are difficult to detect and our understanding of the factors that control their lifetime and radiative properties is limited by a lack of observations. This study demonstrates that spectrally resolved measurements of downwelling longwave radiation can be used to generate retrievals of fog microphysical properties (phase and particle effective radius) when the fog visible optical depth is greater than ~0.25. For 12 cases of fog under otherwise clear skies between June and September 2019 at Summit Station in central Greenland, nine cases were mixed-phase. The mean ice particle (optically-equivalent sphere) effective radius was 24.0 ± 7.8 µm, and the mean liquid droplet effective radius was 14.0 ± 2.7 µm. These results, combined with measurements of aerosol particle number concentrations, provide evidence supporting the hypotheses that (a) low surface aerosol particle number concentrations can limit fog liquid water path, (b) fog can act to increase near-surface aerosol particle number concentrations through enhanced mixing, and (c) multiple fog events in quiescent periods gradually deplete near-surface aerosol particle number concentrations.

54 ENVIRONMENTAL SCIENCES↗

Assessing effective radiative forcing from aerosol–cloud interactions over the global ocean

How clouds respond to anthropogenic sulfate aerosols is one of the largest sources of uncertainty in the radiative forcing of climate over the industrial era. This uncertainty limits our ability to predict equilibrium climate sensitivity (ECS)—the equilibrium global warming following a doubling of atmospheric CO 2 . Here, we use satellite observations to quantify relationships between sulfate aerosols and low-level clouds while carefully controlling for meteorology. We then combine the relationships with estimates of the change in sulfate concentration since about 1850 to constrain the associated radiative forcing. We estimate that the cloud-mediated radiative forcing from anthropogenic sulfate aerosols is − 1.11 ± 0.43 W m −2 over the global ocean (95% confidence). This constraint implies that ECS is likely between 2.9 and 4.5 K (66% confidence). Our results indicate that aerosol forcing is less uncertain and ECS is probably larger than the ranges proposed by recent climate assessments.

54 ENVIRONMENTAL SCIENCES↗

Characteristics and sources of fluorescent aerosols in the central Arctic Ocean

The Arctic is sensitive to cloud radiative forcing. Due to the limited number of aerosols present throughout much of the year, cloud formation is susceptible to the presence of cloud condensation nuclei and ice nucleating particles (INPs). Primary biological aerosol particles (PBAP) contribute to INPs and can impact cloud phase, lifetime, and radiative properties. We present yearlong observations of hyperfluorescent aerosols (HFA), tracers for PBAP, conducted with a Wideband Integrated Bioaerosol Sensor, New Electronics Option during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition (October 2019–September 2020) in the central Arctic. We investigate the influence of potential anthropogenic and natural sources on the characteristics of the HFA and relate our measurements to INP observations during MOSAiC. Anthropogenic sources influenced HFA during the Arctic haze period. But surprisingly, we also found sporadic “bursts” of HFA with the characteristics of PBAP during this time, albeit with unclear origin. The characteristics of HFA between May and August 2020 and in October 2019 indicate a strong contribution of PBAP to HFA. Notably from May to August, PBAP coincided with the presence of INPs nucleating at elevated temperatures, that is, >–9°C, suggesting that HFA contributed to the “warm INP” concentration. The air mass residence time and area between May and August and in October were dominated by the open ocean and sea ice, pointing toward PBAP sources from within the Arctic Ocean. As the central Arctic changes drastically due to climate warming with expected implications on aerosol–cloud interactions, we recommend targeted observations of PBAP that reveal their nature (e.g., bacteria, diatoms, fungal spores) in the atmosphere and in relevant surface sources, such as the sea ice, snow on sea ice, melt ponds, leads, and open water, to gain further insights into the relevant source processes and how they might change in the future.

54 ENVIRONMENTAL SCIENCES↗

Experimental and Computational Characterization of a Modified Sioutas Cascade Impactor for Respirable Radioactive Aerosols

Oak Ridge National Laboratory is collecting and characterizing aerosols released when spent nuclear fuel (SNF) rods are fractured in bending. An aerosol collection system was designed and tested to collect respirable sized (<10 μm aerodynamic diameter [AED]) particulates inside a hot cell facility. The setup is a modified version of the commercially available Sioutas cascade impactor, to which additional stages were added to expand the aerosol collection range from 2.5 to ~15 μm AED. To accommodate the additional stages and specific test conditions, the operating flow rate for aerosol collection was reduced, and testing was conducted by using pressure drop measurements, surrogate dust collection, and particle size characterization. The fluid flow distribution within the cascade and its stages was simulated in STAR-CCM+, and the stage-wise pressure drops obtained using the computational fluid dynamics model were then compared to experimental data. Lagrangian particle simulations were also performed, and stage-wise collection statistics were obtained from the simulation for comparison with the experimental data obtained using SNF-surrogate dust particles. The results provide valuable insights into the stage-wise particle collection characteristics of the modified cascade impactor and can also be used to improve the prediction accuracy of the manufacturer-determined analytical correlations.

aerosol modeling↗

Impact of Aerosol and Cloud on the Solar Energy Potential over the Central Gangetic Himalayan Region

We examine the impact of atmospheric aerosols and clouds on the surface solar radiation and solar energy at Nainital, a high-altitude remote location in the central Gangetic Himalayan region (CGHR). For this purpose, we exploited the synergy of remote-sensed data in terms of ground-based AERONET Sun Photometer and satellite observations from the MODerate Resolution Imaging Spectroradiometer (MODIS) and the Meteosat Second Generation (MSG), with radiative transfer model (RTM) simulations and 1 day forecasts from the Copernicus Atmosphere Monitoring Service (CAMS). Clouds and aerosols are one of the most common sources of solar irradiance attenuation and hence causing performance issues in the photovoltaic (PV) and concentrated solar power (CSP) plant installations. The outputs of RTM results presented with high accuracy under clear, cloudy sky and dust conditions for global horizontal (GHI) and beam horizontal irradiance (BHI). On an annual basis the total aerosol attenuation was found to be up to 105 kWh m –2 for the GHI and 266 kWh m –2 for BHI, respectively, while the cloud effect is much stronger with an attenuation of 245 and 271 kWh m –2 on GHI and BHI. The results of this study will support the Indian solar energy producers and electricity handling entities in order to quantify the energy and financial losses due to cloud and aerosol presence.

54 ENVIRONMENTAL SCIENCES↗

Dry and warm conditions in Australia exacerbated by aerosol reduction in China

A substantial decline in anthropogenic aerosols in China has been observed since the initiation of clean air actions in 2013. This study reveals a linkage between aerosol reductions in China and drier and warmer conditions in Australia. Aerosol decline in China trigger alterations in temperature and pressure gradients between the two hemispheres, leading to intensified outflow from Asia towards the South Indian Ocean, strengthening the Southern Indian Subtropical High and its related Southern Trade Winds. Consequently, this atmospheric pattern results in a moisture divergence over Australia. The reduction in surface moisture further results in more surface energy being converted into sensible heat instead of evaporating as latent heat, warming the near-surface air. The intensified dry and warm climate conditions further cause the increase in wildfire risks during fire seasons in Australia. Our study illuminates the potential impact of distant aerosols on precipitation and temperature variations in Australia, offering valuable insights for drought and wildfire risk mitigation in Australia.

aerosol-cloud interaction↗

Burning conditions and transportation pathways determine biomass-burning aerosol properties in the Ascension Island marine boundary layer

Abstract. African biomass-burning aerosol (BBA) in the southeast Atlantic Ocean (SEA) marine boundary layer (MBL) is an important contributor to Earth's radiation budget, yet its representation remains poorly constrained in regional and global climate models. Data from the Layered Atlantic Smoke Interactions with Clouds (LASIC) field campaign on Ascension Island (7.95° S, 14.36° W) provide insight into how burning conditions, fuel type, transport pathways, and atmospheric processing affect the chemical, microphysical, and optical properties of BBA between June and September 2017. A total of 10 individual plume events characterize the seasonal evolution of the BBA properties. Early-season inefficient fires, determined by low refractory black carbon to above-background carbon monoxide mixing ratios (rBC : ΔCO), led to enhanced concentrations of organic- and sulfate-rich aerosols. Mid-season efficient fires, determined by higher rBC : ΔCO values, led to rBC-enriched BBA. A mix of efficient and inefficient fires later in the season resulted in conflicting BBA properties. Prolonged transport (∼ 10 d) through the MBL and lower free troposphere (FT) facilitated chemical and aqueous-phase processing, which led to a reduction in organic aerosol mass concentrations. This resulted in lower organic aerosol (OA) to rBC (OA : rBC) mass ratios (2–5) in the MBL compared to higher values (5–15) in the nearby FT. These atmospheric and cloud oxidation processes yield more light-absorbing BBA and explain the notably low single-scattering albedo at 530 nm (SSA530) values (< 0.80) observed in the MBL. This study establishes a robust correlation between SSA530 and OA : rBC across the MBL and FT, underscoring the dependency of optical properties on chemical composition.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

BSEC Air Quality: Stationary Aerosol Composition and Mass Concentration at Baltimore

Data is 10-min average mass composition and mass concentration from the TOF-ACSM-X and Aethalometer AE33. TOF-ACSM-X reports fine (less than 2.5 um diameter) non-refractory aerosol, including organic aerosol, sulfate, nitrate, ammonium, and non-refractory chloride. Aethalometer measured the attenuation at different wavelengths for aerosol collected onto tape; one wavelength is used to convert to black carbon mass concentration. Also reported is the elemental ratios determined for organic aerosol (O/C, H/C, and organic matter to organic carbon ratio, OM/OC).

aerosol↗

Enhanced Deep Blue Aerosol Retrieval Algorithm: The Second Generation

The aerosol products retrieved using the MODIS collection 5.1 Deep Blue algorithm have provided useful information about aerosol properties over bright-reflecting land surfaces, such as desert, semi-arid, and urban regions. However, many components of the C5.1 retrieval algorithm needed to be improved; for example, the use of a static surface database to estimate surface reflectances. This is particularly important over regions of mixed vegetated and non- vegetated surfaces, which may undergo strong seasonal changes in land cover. In order to address this issue, we develop a hybrid approach, which takes advantage of the combination of pre-calculated surface reflectance database and normalized difference vegetation index in determining the surface reflectance for aerosol retrievals. As a result, the spatial coverage of aerosol data generated by the enhanced Deep Blue algorithm has been extended from the arid and semi-arid regions to the entire land areas.

Deep Blue↗

Observation and Quantification of Aerosol Outflow from Southern Africa Using Spaceborne Lidar

Biomass burning in Africa provides a prolific source of aerosols that are transported from the source region to distant areas, as far away as South America and Australia. Models have long predicted the primary outflow and transport routes. Over time, field studies have validated the basic production and dynamics that underlie these transport patterns. In more recent years, the advancement of spaceborne active remote sensing techniques has allowed for more detailed verification of the models and, importantly, verification of the vertical distribution of the aerosols in the transport regions, particularly with respect to westerly transport over the Atlantic Ocean. The Cloud-Aerosol Transport System (CATS) lidar on the International Space Station has detection sensitivity that provides observations that support long-held theories of aerosol transport from the African subcontinent over the remote Indian Ocean and as far downstream as Australia.

Lidar↗