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At least 37 records · Page 2

Physicochemical and Molecular Insights into the Boundary Layer and Free Troposphere Aerosol Interactions over the Southern Great Plains

Ambient aerosols’ vertical profiles are critical for evaluating the role of aerosols in atmospheric chemistry and radiative transfer, but limited data on these profiles hinders our ability to fully assess their impact on the Earth's radiative balance. Here, in this study, we investigated the size-, time-, and altitude resolved composition of individual particles and bulk molecular composition of particle samples collected by an uncrewed aerial system–ArcticShark over the Southern Great Plains. Single particle microanalysis shows that, the free tropospheric (FT) samples are dominated (56-66%) by carbonaceous sulfate particles, while boundary layer (BL) samples are dominated (57-74%) by carbonaceous particles. Back trajectory simulations suggest that FT particles are likely influenced by long-range transport and have undergone aqueous-phase processing. Conversely, in-situ size distribution data shows evidence of particle growth in the upper BL and just below the FT. This observation may indicate vertical transport of particles from an elevated aerosol layer in the FT, possibly linked to a new particle formation event. This observation is further supported by high resolution molecular composition data, which reveals particle volatility increasing with increasing size, which aligns with the growth event. This study aids in fundamental understanding of the compositional and molecular specificity of vertically resolved organic aerosols to provide insights into particle size evolution for future atmospheric models.

ArcticShark

Aerosol Optical Properties as Part of the Long-Term Aerosol Measurements in Puerto Rico (AOP-LAMP) Field Campaign Report

The University of Puerto Rico-Rio Piedras Campus (UPR-RP) has been measuring aerosol optical, chemical, and microphysical properties at Cape San Juan (CSJ, also known as CPR) since 2004. This site has also hosted several intensive field campaigns, with context provided by the long-term measurements. Hurricane Maria largely destroyed the station on September 20, 2017, forcing a cessation of the measurements. The scientific focus of this intensive operational period was to use a U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Mobile Facility (AMF) aerosol shelter to enable the resumption of long-term aerosol measurements. This AMF shelter is now the main aerosol shelter for CSJ operations.

54 ENVIRONMENTAL SCIENCES

Developing A Custom-Built Metal Aerosol Processing Chamber: Analysis of Aerosol Coagulation at Low Humidities

We have developed an intermediate size (906 L) aerosol processing chamber, and this work reports on the design and initial characterization of dry aerosol experiments. Specifically, we are determining wall-loss and coagulation correction factors using the observed size distribution measurements for surrogates of common aerosol classes: sodium chloride, sucrose, and biomass burning aerosol smoke. Results show that, on average, sodium chloride, sucrose, and smoke wall-loss rates converge to similar values on relatively short time scales (< 1 h). The fitted coagulation correction factor, W C -1 , for smoke particles (1.23 ± 0.312), indicates that on average they adhere to each other more than sodium chloride (0.969 ± 0.524) and sucrose (1.16 ± 1.38). The relative uncertainty is high for the coagulation correction, but it is consistent with our Monte Carlo error analysis. This study lays the foundation for future experiments at elevated humidity and supersaturation conditions to characterize the influence of particle shape on coagulation and cloud parameters.

54 ENVIRONMENTAL SCIENCES

Implications of stratospheric aerosol measurements for models of aerosol formation and evolution

Calculations of the distribution of stratospheric sulfur gases and of stratospheric aerosols are compared with measurements obtained in Alaska during July 1979. Generally, the measurements are reasonably consistent with the model results. COS is the major sulfur-bearing gas in the stratosphere while CS2 plays a lesser role in the formation of sulfate aerosols. Ammonia, which earlier measurements suggested was a major aerosol constituent, is found to be a contaminant, so models without ammonia chemistry may be justified. The model and the measurements suggest that stratospheric sulfuric acid aerosols nucleate just above the tropopause, but they are older and have grown to larger sizes at higher altitudes.

Toon, O. B.

Investigating ultrafine aerosol turbulent fluxes during atmospheric new particle formation events

New particle formation (NPF) is an important source of atmospheric aerosols, yet quantitatively predicting its occurrence remains challenging, partly because ground-based measurements cannot capture NPF accurately if they occur in the upper atmosphere. While observations have confirmed the presence of new particles near the top of the planetary boundary layer (PBL), their origins and the direction of their vertical transport have remained ambiguous. Here, we propose and validate an analytical framework using airborne eddy-covariance (EC) and continuous wavelet transform (CWT) to directly quantify the vertical flux of newly formed particles and determine its dominant vertical transportation direction. Analyzing data from a dedicated airborne campaign over the Southern Great Plains, we observed a persistent and strong downward particle flux during NPF events, with a mean value of 133.8 cm?3 m s?¹ downward flux in the entrainment zone, whereas fluxes on non-NPF days were negligible. Our spectral analysis further confirms that these directional fluxes can be reliably captured using standard 1 Hz aerosol instrumentation. These findings suggest that new particle formation, driven by the entrainment of air from the overlying residual/stable layer during PBL growth, is a significant and potentially understudied source of boundary layer aerosols. The framework presented here provides a methodology to correctly attribute NPF events to specific altitudes, thereby improving the mechanistic understanding required for accurate atmospheric models.

Zhang, Ruoyu

Kinetic Modeling of Secondary Organic Aerosol in a Weather-Chemistry Model: Parameterizations, Processes, and Predictions for GOAmazon

Secondary organic aerosol (SOA) forms and evolves in the atmosphere through many pathways and processes, over diverse spatial and time scales. Hence, there is a need to represent these widely-varying kinetic processes in large-scale atmospheric models to allow for accurate predictions of the abundance, properties, and impacts of SOA. In this work, we integrated a kinetic, process-level model (simpleSOM-MOSAIC) into a weather-chemistry model (WRF-Chem) to simulate the oxidation chemistry and microphysics of atmospheric SOA. simpleSOM-MOSAIC simulates multigenerational gas-phase chemistry, autoxidation reactions, heterogeneous oxidation, oligomerization, and phase-state-influenced gas/particle partitioning of SOA. As a case study, the integrated WRF-Chem-simpleSOM-MOSAIC (WC-SSM) model was used to simulate the photochemical evolution downwind of a large city (Manaus, Brazil) in the Amazon and, in turn, study the anthropogenic and biogenic interactions in an otherwise pristine environment. Consistent with previous work, we found that OA was enhanced by up to a factor of four in the urban plume due to elevated hydroxyl radical (OH) concentrations, relative to the background, and that this OA was dominated by SOA from biogenic precursors (80%). Further, in addition to accurately simulating the OA enhancement in the urban plume, the model reproduced the magnitude of the OA oxygen-to-carbon (O:C) ratio and broadly tracked the evolution of the aerosol size distribution. Our work highlights the importance of including an integrated, kinetic representation of SOA processes in an atmospheric model

54 ENVIRONMENTAL SCIENCES

Can we mitigate tropical cyclone formation using aerosols? A review of cyclogenesis and aerosol effects as a theoretical basis

Tropical cyclogenesis is a complex phenomenon, involving processes across multiple scales, with various theories proposed to explain its mechanisms. This paper provides an up-to-date summary of the established physical mechanisms and controlling factors of cyclogenesis. Understanding the nature of tropical cyclone formation is necessary to improve tropical cyclone forecasts and inform tropical cyclone mitigation strategies targeting early-stage intervention. Despite the disparities among theories, the critical role of persistent, intensified convection in tropical cyclone initiation is universally acknowledged. Therefore, our hypothesis is that interrupting convective development using aerosol injection is a potential strategy for mitigating tropical cyclone formation. Targetted injection of coarse and fine aerosols at the formation stage are two proposed potential approaches for mitigating tropical cyclones. These methods have completely different microphysical effects but each may ultimately interfere with the formation of the nascent cyclone. In conclusion, these potential interventions open new areas of further research, which are important and necessary to establish a solid scientific foundation for cyclogenesis mitigation.

Tropical cyclone formation

A worldwide aerosol phenomenology: Elemental and organic carbon in PM 2.5 and PM 10

Elemental carbon (EC), organic carbon (OC), and particulate matter (PM) concentrations in the inhalable (PM 10 ) and fine (PM 2.5 ) size fractions are measured worldwide, albeit with different analytical methods. These measurements from many researchers were collected and analyzed for Africa, America, Asia, and Europe for 2012–2019. EC/PM, OC/PM, and OC/EC ratios were examined based on region, site type, and season to infer potential sources and impacts. These analyses demonstrate that carbonaceous materials are important PM constituents throughout the world. Mean EC/PM ratios were lowest in PM 10 in Sahelian Africa and Europe (∼0.01), highest (>0.07) in PM 2.5 at urban sites in North America, South America, and Japan. Mean OC/PM ratios were lowest in PM 10 in the Sahel (∼0.06) and in PM 2.5 in China and Thailand (0.10), and highest in central and eastern Europe (∼0.3) and North America (∼0.4). OC/EC ratios were elevated in western and northern Europe, and at regional background sites in North America. EC/PM increased with PM 10 in Thailand, while OC/PM increased with higher PM mass in Thailand, India, and North America, highlighting the specific contribution of carbonaceous aerosols to PM pollution in these regions. At European and North American background sites, OC/EC ratios increased with PM mass. Higher OC/EC ratios in dry periods indicate influence of wildfires, prescribed burns, and secondary aerosol formation. Elevated wintertime EC/PM ratios coincide with residential heating in temperate climate zones.

54 ENVIRONMENTAL SCIENCES

Performance of pumped counterflow virtual impactors to study aerosol interactions with laboratory generated warm clouds

Pumped Counterflow Virtual Impactors (PCVI) are designed to separate aerosols based on aerodynamic diameter, which is particularly useful for isolating cloud droplets and ice crystals from smaller particles. However, the PCVI transmission efficiency (TE) values reported in the literature show considerable variability, and little information is available on the TEs for cloud liquid droplets. Here, we determined the optimal flow conditions for PCVI sampling for different activation ratios from the MTU Pi-cloud chamber, highlighting the conditions that maximize droplet residual sampling while minimizing interstitial transmission. Even for a lower limit cloud activation ratio = 1:10, an add flow of 1.5 LPM achieves a residual fraction greater than 0.80, with a droplet TE of ∼15% for typical Pi-Chamber droplets with diameters between 3.5 to 10 µm. This framework can be adapted for field cloud measurements based on the cloud conditions of interest. TE for cloud droplets under flow conditions at which ∼99% of the unactivated submicron particles were removed was substantially lower between 8 and 16% than for supermicron dry particles (∼30 to 40% for 3 µm polystyrene latex spheres). In addition, we conducted a comparison of the performances of three similar PCVI units to assess repeatability for dry aerosols and cloud droplets. All three PCVIs performed similarly in rejecting submicron particles smaller than the desired cutoff diameter. One of the units showed lower TEs due to a misalignment of the internal orifice. We discuss a procedure that improved alignment and performance.

54 ENVIRONMENTAL SCIENCES

OpenCRUMS USA: An Open Machine Learning Framework for Characterizing Variability in Aerosol Reanalysis Data

Advances in artificial intelligence (AI) have called for exploring how these techniques can be used for exploring patterns in large climate datasets. To that regard, the U.S. Department of Energy AI for Earth System Predictability (AI4ESP) supported a pilot initiative called the Open Classification of Regimes in the Southeast USA (OpenCRUMS USA) project to explore how AI can be used to characterize modes of spatial variability in large climate datasets. For this study, we focus on comparing two methods for characterizing the modes of spatial variability of surface aerosol concentration over the Houston region: empirical orthogonal functions (EOFs) and layerwise relevance propagation (LRP) applied to a convolutional neural network (CNN) classifier. We show that EOF analysis typically attributes spatial variability modes that span all of southeast Texas, prohibiting the attribution of spatial variability to localized regions. However, using LRP on the CNN classifier resolves the explanatory parameters at a finer spatial resolution than EOFs. This allows for the attribution of the spatial variability of surface aerosols to local regions of organic carbon which was not possible using EOFs. In addition, the LRP analysis also suggests that synoptic-scale transport of dust is most prevalent during anticyclonic and pretrough synoptic conditions as categorized by self-organizing maps.

54 ENVIRONMENTAL SCIENCES

Vertical distribution of aerosol extinction cross section and inference of aerosol imaginary index in the troposphere by lidar technique

The paper reports on vertical profiles of aerosol extinction and backscatter in the troposphere which were obtained from multi zenith angle lidar measurements. It is reported that a direct slant path solution was found to be not possible due to horizontal inhomogeneity of the atmosphere. Attention is given to the use of a regression analysis with respect to zenith angle for a layer integration of the angle dependent lidar equation in order to determine the optical thickness and aerosol extinction-to-backscatter ratio for defined atmospheric layers and the subsequent evaluation of cross-section profiles.

Spinhirne, J. D.

Implications of reduced-complexity aerosol thermodynamics on organic aerosol mass concentration and composition over North America

Atmospheric organic aerosol (OA) mass concentrations can be affected by water uptake through its impact on the gas–particle partitioning of semi-volatile compounds. Current chemical transport models (CTMs) neglect this process. We have implemented the Binary Activity Thermodynamics model coupled to a volatility basis set partitioning scheme in the GEOS-Chem CTM, providing an efficient reduced-complexity OA model that predicts relative-humidity-dependent mixing and partitioning thermodynamics, while limiting the impact on computational efficiency. We provide a quantitative assessment of this water-sensitive OA treatment, focusing on a subdomain over North America. The updated OA scheme predicts a spatiotemporal mean enhancement in surface-level OA mass concentration of 145 % for January 2019 and 76 % for July 2019 compared to GEOS-Chem's most advanced OA scheme. The temporal mean surface-level OA organic mass concentration can increase by up to ∼590 % for January 2019 and ∼280 % for July 2019, with the greatest enhancements occurring over the ocean. The updated OA scheme also quantifies the OA-associated water content. The simulations show how different OA precursors and related OA surrogates contribute and respond to water uptake, including that due to changes in temperature and relative humidity over the diurnal cycle in selected winter and summer months. These results are independent of future CTM improvements involving updates to chemical reaction schemes and emission inventories. Our water-sensitive OA scheme allows for a better representation of the seasonal and regional variations in OA mass concentration in CTMs.

54 ENVIRONMENTAL SCIENCES