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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.

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At least 1,783 records · Page 99
All sourcesNASA NTRSDOE OSTI
DOE OSTI2015

Effect of heterogeneous aqueous reactions on the secondary formation of inorganic aerosols during haze events

In this study, the effect of heterogeneous aqueous reactions on the secondary formation of inorganic aerosols during haze events was investigated by analysis of comprehensive measurements of aerosol composition and concentrations [e.g., particular matters (PM 2.5 ), nitrate (NO 3 ), sulfate (SO 4 ), ammonium (NH 4 )], gas-phase precursors [e.g., nitrogen oxides (NOx), sulfur dioxide (SO 2 ), and ozone (O 3 )], and relevant meteorological parameters [e.g., visibility and relative humidity (RH)]. The measurements were conducted in Beijing, China from Sep. 07, 2012 to Jan. 16, 2013. The results show that the conversion ratios of N from NOx to nitrate (N ratio ) and S from SO 2 to sulfate (S ratio ) both significantly increased in haze events, suggesting enhanced conversions from NOx and SO 2 to their corresponding particle phases in the late haze period. Further analysis shows that N ratio and S ratio increased with increasing RH, with N ratio and S ratio being only 0.04 and 0.03, respectively, when RH < 40%, and increasing up to 0.16 and 0.12 when RH reached 60–80%, respectively. The enhanced conversion ratios of N and S in the late haze period is likely due to heterogeneous aqueous reactions, because solar radiation and thus the photochemical capacity are reduced by the increases in aerosols and RH. This point was further affirmed by the relationships of N ratio and S ratio to O 3 : the conversion ratios increase with decreasing O 3 concentration when O 3 concentration is lower than <15 ppb but increased with increasing O 3 when O 3 concentration is higher than 15 ppb. The results suggest that heterogeneous aqueous reactions likely changed aerosols and their precursors during the haze events: in the beginning of haze events, the precursor gases accumulated quickly due to high emission and low reaction rate; the occurrence of heterogeneous aqueous reactions in the late haze period, together with the accumulated high concentrations of precursor gases such as SO 2 and NOx, accelerated the formation of secondary inorganic aerosols, and led to rapid increase of the PM 2.5 concentration.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2018

Laser Ablation-Aerosol Mass Spectrometry-Chemical Ionization Mass Spectrometry for Ambient Surface Imaging

Mass spectrometry imaging is becoming an increasingly common analytical technique due to its ability to provide spatially resolved chemical information. In this paper, we report a novel imaging approach combining laser ablation with two mass spectrometric techniques, aerosol mass spectrometry and chemical ionization mass spectrometry, separately and in parallel. Both mass spectrometric methods provide the fast response, rapid data acquisition, low detection limits, and high-resolution peak separation desirable for imaging complex samples. Additionally, the two techniques provide complementary information with aerosol mass spectrometry providing near universal detection of all aerosol molecules and chemical ionization mass spectrometry with a heated inlet providing molecular-level detail of both gases and aerosols. The two techniques operate with atmospheric pressure interfaces and require no matrix addition for ionization, allowing for samples to be investigated in their native state under ambient pressure conditions. We demonstrate the ability of laser ablation-aerosol mass spectrometry-chemical ionization mass spectrometry (LA-AMS-CIMS) to create 2D images of both standard compounds and complex mixtures. Finally, the results suggest that LA-AMS-CIMS, particularly when combined with advanced data analysis methods, could have broad applications in mass spectrometry imaging applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Learning to Simulate Aerosol Dynamics with Graph Neural Networks

Aerosol effects on climate, weather, and air quality depend on characteristics of individual particles, which are tremendously diverse and change in time. Particle-resolved models are the only models able to capture this diversity in particle physiochemical properties, and these models are computationally expensive. As a strategy for accelerating particle-resolved microphysics models, we introduce Graph-based Learning of Aerosol Dynamics (GLAD) and use this model to train a surrogate of the particle-resolved model PartMC-MOSAIC. GLAD implements a Graph Network-based Simulator (GNS), a machine learning framework that has been used to simulate particle-based fluid dynamics models. In GLAD, each particle is represented as a node in a graph, and the evolution of the particle population over time is simulated through learned message passing. Here, we demonstrate our GNS approach on a simple aerosol system that includes condensation of sulfuric acid onto particles composed of sulfate, black carbon, organic carbon, and water. A graph with particles as nodes is constructed, and a graph neural network (GNN) is then trained using the model output from PartMC-MOSAIC. The trained GNN can then be used for simulating and predicting aerosol dynamics over time. Results demonstrate the framework's ability to accurately learn chemical dynamics and generalize across different scenarios, achieving efficient training and prediction times. We evaluate the performance across four scenarios, highlighting the framework's robustness and adaptability in modeling aerosol microphysics and chemistry.

aerosol chemistry dynamics↗
DOE OSTI2020

Effects of Lateral Entrainment Mixing With Entrained Aerosols on Cloud Microphysics

The effects of entrained environment air and aerosols on cloud properties remain a critical yet understudied topic. This study first introduces a new entraining cloud parcel model considering entrained aerosols. With entrained aerosols represented by a newly introduced parameter, the impacts of entrainment rate and entrained aerosols on cloud microphysical properties are investigated. The results here show that the relationships between entrainment rate and cloud microphysical properties are highly nonlinear when the entrained aerosols vary. With the lateral entrainment mixing, a new phenomenon is revealed that the height of maximum parcel supersaturation cannot be reached when the entrainment rate is beyond a certain critical value. This new critical entrainment rate is different from the critical entrainment rate defined by Barahona and Nenes (2007, https://doi.org/10.1029/2007JD008473), beyond which clouds cannot form. This finding has important implications for developing parameterization of droplet activation, which is based primarily on the assumption of the existence of maximum supersaturation.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Wind-Driven and Seasonal Effects on Marine Aerosol Production in the Bellingshausen Sea, Antarctica

We assessed satellite-retrieved marine aerosol in the western Antarctic Peninsula (WAP) across a 12-year period from coarse-mode aerosol optical depth (AOD C ), often used as a proxy for sea spray aerosol (SSA), and marine aerosol optical depth (MAOD), a newly developed proxy for tropospheric marine aerosol. Across open ocean to coastal regions, daily fluctuations in nighttime and daytime winds, respectively, drove increasing MAOD and AOD C . MAOD depicted strong correlations with wind speed across open ocean and weak correlations in coastal regions. In the open ocean, AOD C exhibited a very weak significant correlation to wind speed and a weak significant correlation to sea surface temperature (SST). We thus observed that warmer SST enhanced the production of SSA, supporting prior studies. This is the first study to assess patterns of AOD C in the WAP. In contrast to the tropical Pacific, seasonal patterns showed that biological activity likely contributed toward MAOD and AOD C magnitudes.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Emerging investigator series: influence of marine emissions and atmospheric processing on individual particle composition of summertime Arctic aerosol over the Bering Strait and Chukchi Sea

The Arctic is rapidly transforming due to sea ice loss, increasing shipping activity, and oil and gas development. Associated marine and combustion emissions influence atmospheric aerosol composition, impacting complex aerosol–cloud–climate feedbacks. To improve understanding of the sources and processes determining Arctic aerosol composition, atmospheric particles were collected aboard the Korean icebreaker R/V Araon cruising within the Bering Strait and Chukchi Sea during August 2016. Offline analyses of individual particles by microspectroscopic techniques, including scanning electron microscopy with energy dispersive X-ray spectroscopy and atomic force microscopy with infrared spectroscopy, provided information on particle size, morphology, and chemical composition. The most commonly observed particle types were sea spray aerosol (SSA), comprising ~60–90%, by number, of supermicron particles, and organic aerosol (OA), comprising ~50–90%, by number, of submicron particles. Sulfate and nitrate were internally mixed within both SSA and OA particles, consistent with particle multiphase reactions during atmospheric transport. Within the Bering Strait, SSA and OA particles were more aged, with greater number fractions of particles containing sulfate and/or nitrate, compared to particles collected over the Chukchi Sea. This is indicative of greater pollution influence within the Bering Strait from coastal and inland sources, while the Chukchi Sea is primarily influenced by marine sources.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2015

Electron mean free path from angle-dependent photoelectron spectroscopy of aerosol particles

We propose angle-resolved photoelectron spectroscopy of aerosol particles as an alternative way to determine the electron mean free path of low energy electrons in solid and liquid materials. The mean free path is obtained from fits of simulated photoemission images to experimental ones over a broad range of different aerosol particle sizes. The principal advantage of the aerosol approach is twofold. First, aerosol photoemission studies can be performed for many different materials, including liquids. Second, the size-dependent anisotropy of the photoelectrons can be exploited in addition to size-dependent changes in their kinetic energy. These finite size effects depend in different ways on the mean free path and thus provide more information on the mean free path than corresponding liquid jet, thin film, or bulk data. The present contribution is a proof of principle employing a simple model for the photoemission of electrons and preliminary experimental data for potassium chloride aerosol particles.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

An estimation of impact of anthropogenic aerosols in atmosphere of Tirana on solar insolation. Part II: Modification of solar energy potential

Change of irradiative properties of the atmosphere during clear days is an indicator, among others, of existence of atmospheric aerosols and can be used as an indicator for assessment both air pollution and local modifications of solar energy potentials. The main objective of this study is estimation of influence of anthropogenic aerosols on solar energy falling in a horizontal surface during a cloudless day. We have analyzed and quantified the effect of aerosols on reducing the amount of solar energy that falls on the horizontal ground surface in cloudless sky conditions, estimating temporal evolution, both in daily and hour scale, considering also, side effects caused by relative humidity of the air wind speed and geometric factor. As an indicator of concentration of aerosols in atmosphere, we agreed to use the attenuation of solar radiation after the last rainy day. All data were corrected by factors such as, variations of relative humidity, wind speed and daily change of incident angle of solar radiation. We studied the change of solar insolation in three sites with different traffic intensity, one in city of Shkodra and two in city of Tirana. Fifteen days after last rainy day, approximate time needed to achieve saturation, the insolation drops only 3.1% in the city of Shkodra, while in two sites in city of Tirana are 8.5 % and 18.4%. These data show that reduction of solar insolation is closely related with anthropogenic activity, mainly traffic around the site of the meteorological station. The day to day difference tends to decrease with increasing of number of days passed from the last rainy day, which is an evidence of a trend toward a dynamic equilibrium between decantation process of aerosols during the night and their generation during the day.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Tropical African wildfire aerosols trigger teleconnections over mid-to-high latitudes of Northern Hemisphere in January

This study investigates the impacts of African wildfire aerosols (primary organic carbon, black carbon and sulfate) on the Northern Hemispheric in January. We found that wildfire aerosols emitted from equatorial Africa result in two mid-to-high latitudes atmospheric Rossby wave trains. One is from subtropical Atlantic propagating northeastward across Europe to Siberia, and the other one propagates eastward from Middle East across Asia to Pacific Northwest. The maximum positive geopotential height anomaly locates in Europe, concurrent with a greater-than-2 K land surface warming. These Rossby wave trains are excited by the atmospheric heating that caused by the wildfire aerosols in equatorial Africa and propagate into extratropics with the help of the westerly jet. Based on the diabatic heat budget analysis, the Rossby wave source is primarily from the solar absorption of black carbon of African wildfire. The present study emphasizes that wildfire aerosols, especial the absorbing aerosols, would have profound climate effects on remote regions and thus need more attentions.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Anthropogenic aerosols prolong fog lifetime in China

Investigation of aerosol effects on fog with long-term measurements has generally focused on fog occurrence frequency and intensity; here we examine the effects on fog lifetime, fog formation, and fog dissipation. From analysis of 52 years (1960–2011) of data collected at 404 stations in China, it is found that fog lifetime exhibits a clear increasing trend with time, and the increased lifetime is mainly attributable to delayed fog dissipation. Increased aerosol levels and global warming affect fog lifetime in opposite ways; increased aerosol levels serve to prolong fog lifetime by primarily delaying fog dissipation, whereas warming decreases fog lifetime by primarily delaying fog formation. The overall aerosol effect on fog lifetime in China is shown to predominate, especially in the highly polluted region of Eastern China. The observational findings are confirmed by a suite of WRF-Chem simulations that reveal the influences of both increased aerosol levels and temperatures through a complex chain of interactions among microphysical, dynamical, thermodynamic, and radiative processes.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2026

The role of local shipping emissions in aerosol-cloud interactions in the central Arctic

Arctic shipping is projected to increase as sea ice retreats, yet the impact of modern low-sulfur ship emissions on Arctic clouds and radiation remain poorly constrained. We use year-long in situ observations from the MOSAiC expedition to characterize ship-aerosol-cloud interactions for an icebreaker burning ultra-low sulfur fuel (0.1% mass per mass). Exhaust plumes were found to be strongly enriched in Aitken-mode particles, organic aerosol, and black carbon, but showed no detectable enhancement in particulate sulfate. Despite reduced hygroscopicity relative to ambient aerosols, ship emissions substantially increased local cloud condensation nuclei concentrations. A droplet activation parameterization was applied to quantify responses in cloud droplet number concentration ( N d ) to ship-induced perturbations in low-level Arctic clouds. In winter, abundant background accumulation-mode particles from Arctic haze supplied nearly all cloud droplets, while additional particles from ship emissions had little impact on N d . In contrast, during summer months, when unperturbed background aerosol concentrations are low, ship emissions nearly doubled N d compared to average background conditions and increased N d by a factor of five compared to very clean background conditions (25th percentile of background aerosol number concentrations). Longwave radiative transfer simulations for typical conditions of summer Arctic low-level clouds/fog suggest that these ship-induced increases in N d locally (i.e. <100 km downwind) lead to enhanced net surface longwave fluxes and consequent warming, primarily for optically thin clouds (liquid water path (LWP) ⩽ 30 g·m −2 ). For LWP = 10 g · m −2 , ship emissions lead to an increase of 1 W · m −2 in cloud longwave forcing at the surface compared to average unperturbed conditions (+7% relative increase), and up to 4 W · m −2 when compared to very clean background conditions (+22% relative increase). Even ultra-low sulfur fuel emissions can therefore locally and episodically modify Arctic cloud microphysics and radiative properties, especially during summer, implying that future increases in Arctic shipping could have non-negligible regional climate impacts.

Arctic↗
DOE OSTI2016

ARM-Led Improvements Aerosols in Climate and Climate Models

The DOE ARM program has played a foundational role in efforts to quantify aerosol effects on climate, beginning with the early back-of-the-envelope estimates of direct radiative forcing by anthropogenic sulfate and biomass burning aerosol (Penner et al., 1994). In this chapter we review the role that ARM has played in subsequent detailed estimates based on physically-based representations of aerosols in climate models. The focus is on quantifying the direct and indirect effects of anthropogenic aerosol on the planetary energy balance. Only recently have other DOE programs applied the aerosol modeling capability to simulate the climate response to the radiative forcing.

aerosol↗
DOE OSTI2021

Observations of Clouds, Aerosols, Precipitation, and Surface Radiation over the Southern Ocean: An Overview of CAPRICORN, MARCUS, MICRE, and SOCRATES

Weather and climate models are challenged by uncertainties and biases in simulating Southern Ocean (SO) radiative fluxes that trace to a poor understanding of cloud, aerosol, precipitation, and radiative processes, and their interactions. Projects between 2016 and 2018 used in situ probes, radar, lidar, and other instruments to make comprehensive measurements of thermodynamics, surface radiation, cloud, precipitation, aerosol, cloud condensation nuclei (CCN), and ice nucleating particles over the SO cold waters, and in ubiquitous liquid and mixed-phase clouds common to this pristine environment. Data including soundings were collected from the NSF–NCAR G-V aircraft flying north–south gradients south of Tasmania, at Macquarie Island, and on the R/V Investigator and RSV Aurora Australis. Synergistically these data characterize boundary layer and free troposphere environmental properties, and represent the most comprehensive data of this type available south of the oceanic polar front, in the cold sector of SO cyclones, and across seasons. Results show largely pristine environments with numerous small and few large aerosols above cloud, suggesting new particle formation and limited long-range transport from continents, high variability in CCN and cloud droplet concentrations, and ubiquitous supercooled water in thin, multilayered clouds, often with small-scale generating cells near cloud top. These observations demonstrate how cloud properties depend on aerosols while highlighting the importance of dynamics and turbulence that likely drive heterogeneity of cloud phase. Satellite retrievals confirmed low clouds were responsible for radiation biases. Furthermore, the combination of models and observations is examining how aerosols and meteorology couple to control SO water and energy budgets.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Quantification of the Radiative Effect of Aerosol–Cloud Interactions in Shallow Continental Cumulus Clouds

The indirect radiative effect of aerosol variability on shallow cumulus clouds is realized in nature with considerable concurrent meteorological variability. Large-eddy simulations constrained by observations at a continental site in Oklahoma are performed to represent the variability of different meteorological states on days with different aerosol conditions. The total radiative effect of this natural covariation between aerosol and other meteorological drivers of total cloud amount and albedo is quantified. The changes to these bulk quantities are used to understand the response of the cloud radiative effect to aerosol–cloud interactions (ACI) in the context of concurrent processes, as opposed to attempting to untangle the effect of individual processes on a case-by-case basis. Mutual information (MI) analysis suggests that meteorological variability masks the strength of the relationship between cloud drop number concentration and the cloud radiative effect. This is shown to be mostly due to variation in solar zenith angle and cloud field horizontal heterogeneity masking the relationship between cloud drop number and cloud albedo. By combining MI and more traditional differential analyses, a framework to identify important modes of covariation between aerosol, clouds, and meteorological conditions is developed. This shows that accounting for solar zenith angle variation and implementing an albedo bias correction increases the detectability of the radiative effects of ACI in simulations of shallow cumulus.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Responses in the Subpolar North Atlantic in Two Climate Model Sensitivity Experiments with Increased Stratospheric Aerosols

Abstract The subpolar North Atlantic (SPNA) shows contrasting responses in two sensitivity experiments with increased stratospheric aerosols, offering insight into the physical processes that may impact the Atlantic meridional overturning circulation (AMOC) in a warmer climate. In one, the upper ocean becomes warm and salty, but in the other it becomes cold and fresh. The changes are accompanied by diverging AMOC responses. The first experiment strengthens the AMOC, opposing the weakening trend in the reference simulation. The second experiment shows a much smaller impact. Both simulations use the Community Earth System Model with the Whole Atmosphere Community Climate Model component (CESM-WACCM) but differ in model versions and stratospheric aerosol specifications. Despite both experiments using similar approaches to increase stratospheric aerosols to counteract the rising global temperature, the contrasting SPNA and AMOC responses indicate a considerable dependency on model physics, climate states, and model responses to forcings. This study focuses on examining the physical processes involved with the impact of stratospheric aerosols on the SPNA salinity changes and their potential connections with the AMOC and the Arctic. We find that in both cases, increased stratospheric aerosols act to enhance the SPNA upper-ocean salinity by reducing freshwater export from the Arctic, which is closely tied to the Arctic sea ice changes. The impact on AMOC is primarily through the thermal component of the surface buoyancy fluxes, with negligible contributions from the freshwater component. These experiments shed light on the physical processes that dictate the important connections between the SPNA, the Arctic, the AMOC, and their subsequent feedbacks on the climate system.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2016

Evolution of Aerosol Research in India and the RAWEX–GVAX:An Overview

Climate change has great significance in Asia in general, and India in particular; and atmospheric aerosols have a decisive role in this. The climate forcing potential of aerosols is closely linked to their optical, microphysical and chemical properties. Systematic efforts to characterize these properties over the Indian region started about 5 decades ago, and evolved over the years through concerted efforts in the form of long-term scientific programmes as well as concerted fields experiments. All these have resulted in this activity becoming one of the most vibrant fields of climate research in India and have brought several important issues in the national and international foci. The field experiment, RAWEX-GVAX (Regional Aerosol Warming Experiment-Ganges Valley Aerosol Experiment), conducted during 2011-12 jointly by the US Department of Energy, Indian Space Research Organization and Department of Science and Technology, has emerged as a direct outcome of the above efforts. This overview provides a comprehensive account of the development of aerosol-climate research in India and south Asia, and the accomplishment and newer issues that warranted the above field campaign. Details of RAWEX-GVAX, the major outcomes and the subsequent and more recent efforts are presented, followed by the way forward in this field for the next several years to come.

Aerosols↗
DOE OSTI2015

Synthesis of Aerosol Observations for Improved Understanding of Radiative Forcing

The ultimate objective of this project was to gain a better understanding of the relationship between aerosol physical and radiative properties through the integration of measurements from different approaches and platforms. Different types of information can only be gained from different approaches – for example, in situ sampling versus remote sensing – so to provide the best radiative forcing estimates they must be brought together in accurate and meaningful ways. This work involved understanding and characterizing measurement accuracy, integrating measurements from different approaches, and understanding the sensitivity of different aerosol representations from these various approaches to radiative forcing. Our progress involved the assessment of error and bias in aerosol absorption measurements made in situ and by remote sensing, assessment of new chemical composition measurements made by ARM, and determination of the sensitivity of radiative forcing to these measurement errors and the representation of absorption vertical distributions. We also examined the sensitivity of cloud condensation nuclei, cloud microphysics, and cloud radiative forcing to aerosol concentration, microphysical, chemical, and optical properties, and vertical distributions in distinct aerosol regimes.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2016

Laboratory Experiments and Modeling for Interpreting Field Studies of Secondary Organic Aerosol Formation Using an Oxidation Flow Reactor

This grant was originally funded for deployment of a suite of aerosol instrumentation by our group in collaboration with other research groups and DOE/ARM to the Ganges Valley in India (GVAX) to study aerosols sources and processing. Much of the first year of this grant was focused on preparations for GVAX. That campaign was cancelled due to political reasons and with the consultation with our program manager, the research of this grant was refocused to study the applications of oxidation flow reactors (OFRs) for investigating secondary organic aerosol (SOA) formation and organic aerosol (OA) processing in the field and laboratory through a series of laboratory and modeling studies. We developed a gas-phase photochemical model of an OFR which was used to 1) explore the sensitivities of key output variables (e.g., OH exposure, O 3 , HO 2 /OH) to controlling factors (e.g., water vapor, external reactivity, UV irradiation), 2) develop simplified OH exposure estimation equations, 3) investigate under what conditions non-OH chemistry may be important, and 4) help guide design of future experiments to avoid conditions with undesired chemistry for a wide range of conditions applicable to the ambient, laboratory, and source studies. Uncertainties in the model were quantified and modeled OH exposure was compared to tracer decay measurements of OH exposure in the lab and field. Laboratory studies using OFRs were conducted to explore aerosol yields and composition from anthropogenic and biogenic VOC as well as crude oil evaporates. Various aspects of the modeling and laboratory results and tools were applied to interpretation of ambient and source measurements using OFR. Additionally, novel measurement methods were used to study gas/particle partitioning. The research conducted was highly successful and details of the key results are summarized in this report through narrative text, figures, and a complete list of publications acknowledging this grant.

54 ENVIRONMENTAL SCIENCES↗