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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 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Detecting tropospheric composition and climate responses to US air pollution controls in the context of internally-arising variability

Since the 1970s, air pollutant emissions controls in the United States (US) have lowered concentrations of ozone (O 3 ) and aerosols, which have opposing radiative effects on surface temperature. Using a pair of initial-condition ensembles generated by a fully-coupled chemistry-climate model, we simulate the “world avoided” by US air pollution controls. In this counterfactual world, we find tropospheric column O 3 increases, robust to natural internal variability, extending across the Northern Hemisphere. Robust aerosol increases, dominated by sulfate, remain localized near the US. Wintertime Northwest Atlantic cloud droplet number concentration is particularly sensitive to US aerosol. While an ensemble mean US surface cooling signal (−0.4 °C) implies that aerosol-driven cooling prevails over any O 3 -induced warming, we find that large regional internal variability will confound its detection in any single transient realization. Larger signal-to-noise ratios for composition versus climate variables underscore the greater detectability of emissions-driven changes in tropospheric composition compared to their associated climate impacts.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Ambient Aerosol Is Physically Larger on Cloudy Days in Bondville, Illinois

Particle chemical composition affects aerosol optical and physical properties in ways important for the fate, transport, and impact of atmospheric particulate matter. For example, hygroscopic constituents take up water to increase the physical size of a particle, which can alter the extinction properties and atmospheric lifetime. At the collocated AERosol RObotic NETwork (AERONET) and Interagency Monitoring of PROtected Visual Environments (IMPROVE) network monitoring stations in rural Bondville, Illinois, we employ a novel cloudiness determination method to compare measured aerosol physicochemical properties on predominantly cloudy and clear sky days from 2010 to 2019. On cloudy days, aerosol optical depth (AOD) is significantly higher than on clear sky days in all seasons. Measured angstrom ngstro''m exponents are significantly smaller on cloudy days, indicating physically larger average particle size for the sampled populations in all seasons except winter. Mass concentrations of fine particulate matter that include estimates of aerosol liquid water (ALW) are higher on cloudy days in all seasons but winter. More ALW on cloudy days is consistent with larger particle sizes inferred from angstrom ngstro''m exponent measurements. Aerosol chemical composition that affects hygroscopicity plays a determining impact on cloudy versus clear sky differences in AOD, angstrom ngstro''m exponents, and ALW. This work highlights the need for simultaneous collocated, high-time-resolution measurements of both aerosol chemical and physical properties, in particular at cloudy times when quantitative understanding of tropospheric composition is most uncertain.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

A Succession of Cloud, Precipitation, Aerosol and Air Quality Field Experiments in the Coastal Urban Environment

The interactions and feedbacks among clouds, aerosols, pollutants, and the thermodynamic and kinematic environment remains an area of active research with important implications for our understanding of climate, weather and air quality. These linkages are further complicated in coastal and urban environments where local circulations and anthropogenic influences impact each of these components and their interactions. Within this context, fundamental questions regarding the lifecycle of convective clouds, aerosols and pollutants have brought together a diverse, integrated, and interagency collaboration of scientists to collect and analyze measurements, in the Houston, Texas, area, from the summer of 2021 through the summer of 2022, with subsequent modeling studies to address these important research objectives. Herein, the U.S. Department of Energy’s Atmospheric Radiation Measurement (ARM) Facility and Atmospheric System Research (ASR) Program, the National Science Foundation’s (NSF) Physical and Dynamic Meteorology Program, the National Aeronautic and Space Administration’s (NASA’s) Tropospheric Composition Research and Health and Air Quality Applied Sciences Programs and the Texas Commission on Environmental Quality (TCEQ) are collaborating on a joint set of field campaigns to study the interactions of cloud, aerosol, and pollutants within the coastal, urban environment. In the Houston area, onshore flow from the Gulf of Mexico and the associated sea breeze circulation generates numerous isolated convective cells, particularly in the summer months, that interact with a variety of urban and industrial emissions.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Differences in fine particle chemical composition on clear and cloudy days

Clouds are prevalent and alter fine particulate matter (PM 2.5 ) mass and chemical composition. Cloud-affected satellite retrievals are subject to higher uncertainty and are often removed from data products, hindering quantitative estimates of tropospheric chemical composition during cloudy times. We examine surface PM 2.5 chemical constituent concentrations in the Interagency Monitoring of PROtected Visual Environments (IMPROVE) network in the United States during cloudy and clear-sky times defined using Moderate Resolution Imaging Spectroradiometer (MODIS) cloud flags from 2010 to 2014 with a focus on differences in particle species that affect hygroscopicity and aerosol liquid water (ALW). Cloudy and clear-sky periods exhibit significant differences in PM 2.5 mass and chemical composition that vary regionally and seasonally. In the eastern US, relative humidity alone cannot explain differences in ALW, suggesting that emissions and in situ chemistry related to anthropogenic sources exert determining impacts. An implicit clear-sky bias may hinder efforts to quantitatively understand and improve representation of aerosol–cloud interactions, which remain dominant uncertainties in models.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

CoURAGE Urban Gas-Phase NH3

1-second Picarro gas-phase ammonia (NH3) measurements were collected as part of a 3-month intensive operation period (IOP) from mid-March through mid-June that was funded by the DOE Biological and Environment Research project in conjunction with the DOE ARM CoURAGE deployment to the greater Baltimore region. To complement the NH3 measurements at the Mt. Airy regional background S2 site, the Picarro G2103 NH3 analyzer was deployed at the urban atmospheric chemistry supersite ( 39.32057 N, 76.6246 W) to be able to compare and contrast urban vs regional NH3 and urban vs regional aerosol physicochemical properties.

Aerosol Acidity↗
DOE OSTI2024

Observational evidence for Criegee intermediate oligomerization reactions relevant to aerosol formation in the troposphere

Criegee intermediates are reactive intermediates that are implicated in transforming the composition of Earth’s troposphere and in the formation of secondary organic aerosol, impacting Earth’s radiation balance, air quality and human health. Yet, direct identification of their signatures in the field remains elusive. Here, from particulate and gas-phase mass-spectrometric measurements in the Amazon rainforest, we identify sequences of masses consistent with the expected signatures of oligomerization of the CH 2 OO Criegee intermediate, a process implicated in ozonolysis-driven aerosol formation. In this study, we assess the potential contributions of oligomerization through laboratory ozonolysis experiments, direct kinetic studies of Criegee intermediate reactions, and high-level theoretical calculations. Global atmospheric models built on these kinetics results indicate that Criegee intermediate chemistry may play a larger role in altering the composition of Earth’s troposphere than is captured in current atmospheric models, especially in areas of high humidity. However, the models still capture only a relatively small fraction of the observed signatures, suggesting considerable underestimates of Criegee intermediate concentrations and reactivity and/or the dominance of other, presently uncharacterized, oxidation mechanisms. Resolving the remaining uncertainties in emission inventories and the effects of atmospheric water vapour on key chemical reactions will be required to definitively assess the role of Criegee intermediate oligomerization reactions.

58 GEOSCIENCES↗
DOE OSTI2021

Aerosol Composition, Mixing State, and Phase State of Free Tropospheric Particles and Their Role in Ice Cloud Formation

The prediction of ice cloud formation in the atmosphere remains challenging. Free tropospheric aerosols can act as ice nucleating particles (INPs), affecting cloud properties and precipitation. The physicochemical properties of free tropospheric particles are modified upon long-range transport by different atmospheric processes. These modifications affect the ice formation potential of individual particles. We investigated free tropospheric particles collected at the remote Pico Mountain Observatory at 2225m a.s.l. in the North Atlantic Ocean using multimodal microspectroscopy and chemical imaging techniques. We probed their ice nucleation activity using an ice nucleation stage interfaced with an environmental scanning electron microscope. Retroplume analysis, chemical imaging, and micro-spectroscopy analysis indicated that the size-resolved chemical composition, mixing state, and phase state of the articles with similar aging times but different transport patterns were substantially different. Relative humidity-dependent glass transition temperatures estimated from meteorological conditions were consistent with the observed organic component of the particles' phase. More viscous (solid and semi-solid-like) particles are more ice active in deposition mode at temperature ranging from 205-220 K than those less viscous particles. Finally, this study provides a better understanding of the phase and mixing state of long range transported free tropospheric aerosols and their role in ice cloud formation.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Sensitivity of deep convection and cross-tropopause water transport to microphysical parameterizations in WRF

Deep convective storms can overshoot the tropopause, thus altering the composition of the stratosphere by vertically transporting tropospheric air. The transport of water vapor and ice particles into a sub-saturated environment can hydrate the stratosphere, with implications for radiative forcing and ozone chemistry. Cloud-resolved models, if employed at high spatial resolutions, are used to probe process-level questions about cross-tropopause deep convective hydration and its controls. There is considerable diversity in model representations of processes associated with water transport and transformation, and the choice of a microphysics scheme affects model skill in simulating deep convective events. This motivates our evaluation of state-of-the-art, as well as widely used standard schemes, in a high spatial- and temporal-resolution framework. Six bulk microphysics schemes were employed in a WRF-LES setup, initialized with a sounding profile representative of a tropopause-overshooting storm. Here, we used an idealized framework to isolate the effect of microphysics on the dominant processes that control the reach of deep convection and stratospheric hydration. All schemes produced the highest reaching updrafts 8-12 hours into the simulation but the strength and persistence of updrafts varied across the schemes; maximum storm heights ranged 9.1-12.6 km across the schemes. Varying microphysics produced large differences in the vertical extent and horizontal aggregation of convection, and an order of magnitude spread in above-tropopause water vapor concentrations.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Processes Associated with Boundary Layer Cloud Ice Phase Precipitation in the High Southern Latitudes (Final Technical Report)

This is a final technical report for DOE Award No. DE-SC0018995. Using data collected during the MARCUS deployment of the 2nd ARM mobile facility, this project sought to address the following scientific questions: 1. What are the conditions that govern phase partitioning in supercooled boundary layer clouds over the high latitude Southern Oceans? 2. To what extent are supercooled mixed phase clouds responsible for the high cloud fractions over the Southern Ocean and do these mixed phase clouds contribute to the model biases in absorbed shortwave radiation? 3. Can the cloud properties and phase partitioning over the Southern Ocean be linked to the underlying aerosol environment? 4. How do the aerosol properties at the surface vary spatially and seasonally over the high latitude Southern Ocean and what processes control these features? 5. How well defined are the atmospheric compositional boundaries between Southern Ocean marine, Antarctic free tropospheric, and Antarctic surface airmasses, and how does this influence the chemistry and physics of the Southern Ocean atmosphere? In this project we published three peer review journal articles that address these questions.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Optical Properties of Individual Tar Balls in the Free Troposphere

Tar balls are brown carbonaceous particles, highly viscous, spherical, amorphous, and light absorbing. They are believed to form in biomass burning smoke plumes during transport in the troposphere. Tar balls are believed to have a significant impact on the Earth’s radiative balance, but due to poorly characterized optical properties, this impact is highly uncertain. Here, we investigate the chemical composition and optical properties of individual tar balls transported in the free troposphere to the Climate Observatory “Ottavio Vittori” on Mt. Cimone, Italy (2165 meters above sea level) using multi-modal micro-spectroscopy. Our results show that tar balls contributed 50% of carbonaceous particles by number in the size range from 0.25 to 1.8 µm. Of those tar balls, 16% were inhomogeneously mixed with other constituents. Using electron energy loss spectroscopy, we retrieved the complex refractive index from 200 to 1200 nm for both inhomogeneously and homogeneously mixed tar balls. We found no significant difference in the average refractive index of inhomogeneously and homogenously mixed tar balls (1.40 - 0.03i, and 1.36 - 0.03i at 550 nm, respectively). Furthermore, we estimated the top of the atmosphere radiative forcing using the Santa Barbara DISORT Atmospheric Radiative Transfer model (SBDART) and found that a layer of only tar balls with an optical depth of 0.1 above vegetation would exert a positive radiative forcing ranging from 2.8 Wm-2 (on a clear sky day) to 9.5 Wm-2 (when clouds are below the aerosol layer). In conclusion, understanding the optical properties of tar balls can help reduce uncertainties associated with the contribution of biomass-burning aerosol in current climate models.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Cloud condensation nuclei activity of internally mixed particle populations at a remote marine free troposphere site in the North Atlantic Ocean

Here, this study reports results from research conducted at the Observatory of Mount Pico (OMP), 2225 m above mean sea level on Pico Island in the Azores archipelago in June and July 2017. We investigated the chemical composition, mixing state, and cloud condensation nuclei (CCN) activities of long-range transported free tropospheric (FT) particles. FLEXible PARTicle Lagrangian particle dispersion model (FLEXPART) simulations reveal that most air masses that arrived at the OMP during the sampling period originated in North America and were highly aged (average plume age > 10 days). We probed size-resolved chemical composition, mixing state, and hygroscopicity parameter ($\mathcal{κ}$) of individual particles using computer-controlled scanning electron microscopy with an energy-dispersive X-ray spectrometer (CCSEM-EDX). Based on the estimated individual particle mass from elemental composition, we calculated the mixing state index, $χ$. During our study, FT particle populations were internally mixed ($χ$ of samples are between 53% and 87%), owing to the long atmospheric aging time. We used data from a miniature Cloud Condensation Nucleus Counter (miniCCNC) to derive the hygroscopicity parameter, $\mathcal{κ}$ CCNC . Combining $\mathcal{κ}$ CCNC and FLEXPART, we found that air masses recirculated above the North Atlantic Ocean with lower mean altitude had higher $\mathcal{κ}$ CCNC due to the higher contribution of sea salt particles. We used CCSEM-EDX and phase state measurements to predict single-particle $\mathcal{κ}$ ($\mathcal{κ}$ CCSEM-EDX ) values, which overlap with the lower range of $\mathcal{κ}$ CCNC measured below 0.15 % SS. Therefore, CCSEM-EDX measurements can be useful in predicting the lower bound of $\mathcal{κ}$, which can be used in climate models to predict CCN activities, especially in remote locations where online CCN measurements are unavailable.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Photochemical reactions on aerosols at West Antarctica: A molecular case-study of nitrate formation among sea salt aerosols

Environmental implications of climate change are complex and exhibit regional variations both within and between the polar regions. The increase of solar UV radiation flux over Antarctica due to stratospheric ozone depletion creates the optimal conditions for photochemical reactions on the snow. Modeling, laboratory, and indirect field studies suggest that snowpack process release gases to the atmosphere that can react on sea salt particles in remote regions such as Antarctica, modifying aerosol composition and physical properties of aerosols. Here, we present evidence of photochemical processing in West Antarctica aerosols using microscopic and chemical speciation of individual atmospheric particles. Individual aerosol particles collected at the Brazilian module Criosfera 1 were analyzed by scanning transmission X-ray microscopy with near edge X-ray absorption fine structure spectroscopy (STXM/NEXAFS) combined with computer controlled scanning electron microscopy (CCSEM) with energy-dispersive X-ray (EDX) microanalysis. The displacement of chlorine relative to sodium was observed over most of the sea salt particles. Particles with a chemical composition consistent with NaCl-NO3 contributed up to 30% of atmospheric particles investigated. Overall, this study provides evidence that the snowpack and particulate nitrate photolysis should be considered in dynamic partition equilibrium in the troposphere. Finally, these findings may assist in reducing modeling uncertainties and present new insights into the aerosol chemical composition in the polar environment.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Particle phase-state variability in the North Atlantic free troposphere during summertime is determined by atmospheric transport patterns and sources

Abstract. Free tropospheric aerosol particles have important but poorly constrained climate effects due to transformations of their physicochemical properties during long-range transport. In this study, we investigate the chemical composition and provide an overview of the phase states of individual particles that have undergone long-range transport over the North Atlantic Ocean in June and July 2014, 2015, and 2017 to the Observatory of Mount Pico (OMP) in the Azores. The OMP is an ideal site for studying long-range-transported free tropospheric particles because local emissions have a negligible influence and contributions from the boundary layer are rare. We used the FLEXible PARTicle Lagrangian particle dispersion model (FLEXPART) to determine the origins and transport trajectories of sampled air masses and found that most of them originated from North America and recirculated over the North Atlantic Ocean. The FLEXPART analysis showed that the sampled air masses were highly aged (average plume age >10 d). Size-resolved chemical compositions of individual particles were probed using computer-controlled scanning electron microscopy with an energy-dispersive X-ray spectrometer (CCSEM-EDX) and scanning transmission X-ray microscopy with near-edge X-ray absorption fine structure spectroscopy (STXM-NEXAFS). CCSEM-EDX results showed that the most abundant particle types were carbonaceous (∼ 29.9 % to 82.0 %), sea salt (∼ 0.3 % to 31.6 %), and sea salt with sulfate (∼ 2.4 % to 31.5 %). We used a tilted stage interfaced within an environmental scanning electron microscope (ESEM) to determine the phase states of individual submicron particles. We found that most particles (∼ 47 % to 99 %) were in the liquid state at the time of collection due to inorganic inclusions. Moreover, we also observed substantial fractions of solid and semisolid particles (∼ 0 % to 30 % and ∼ 1 % to 42 %, respectively) during different transport patterns and events, reflecting the particles' phase-state variability for different atmospheric transport events and sources. Combining phase state measurements with FLEXPART CO tracer analysis, we found that wildfire-influenced plumes can result in particles with a wide range of viscosities after long-range transport in the free troposphere. We also used temperature and RH values extracted from the Global Forecast System (GFS) along the FLEXPART-simulated path to predict the phase state of the particles during transport and found that neglecting internal mixing with inorganics would lead to an overestimation of the viscosity of free tropospheric particles. Our findings warrant future investigation aiming at the quantitative assessment of the influence of internal mixing on the phase states of the individual particles. This study also provides insights into the chemical composition and phase state of free tropospheric particles, which can help models to reduce uncertainties about the effects of ambient aerosol particles on climate.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Upper-Tropospheric Troughs and North American Monsoon Rainfall in a Long-Term Track Dataset

The North American monsoon is frequently affected by transient, propagating upper tropospheric vorticity anomalies. Sometimes called Tropical Upper-Tropospheric Troughs (TUTTs), these features have been claimed to episodically enhance monsoon rainfall. Here, we track long-lived TUTTs in 40 years of reanalysis data, producing composites and case studies from 340 TUTTs which last, on average, 7 days as they move westward across the North American monsoon region. TUTTs are thought to form from midlatitude Rossby wave breaking; case studies from our dataset support this theory. TUTTs move westward within the easterly upper-level flow in which they are embedded. In vortex-centered composites along the full tracks of long-lived TUTTs, here, we find no detectable increase in rainfall within the main TUTT circulation. Instead, negative precipitation anomalies lie within about 500 km of the TUTT center. Quasi-geostrophic ascent occurs in the southeast quadrant of TUTTs but is confined to the upper troposphere and does not appear to interact with precipitation. Positive anomalies of ascent and rainfall occur south and southeast of TUTTs but lie outside the main TUTT vortex, perhaps indicating concurrent variations in nearby climatological precipitation maxima. In contrast with previous case studies and subjective analyses that showed TUTTs enhance precipitation in parts of northwestern Mexico, our composites along the tracks of long-lived TUTTs portray these systems, to first order, as strong vorticity anomalies trapped in the upper troposphere that interact only weakly and indirectly with precipitation.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

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↗
DOE OSTI2026

Deep Convection‐Driven Downward Transport of Trace Gases and Aerosols From the Free Troposphere to the Boundary Layer

Deep convective clouds regulate Earth's energy and moisture budgets, yet their impact on the atmospheric boundary layer (BL) composition remains underexplored. Using long-term observations from three mid-latitude sites, we show that deep convection (DC) consistently enhances nighttime surface ozone and is often accompanied by modest increases in ultrafine particle concentrations. Within the BL, the condensational growth of these transported ultrafine particles may contribute up to 60% of total cloud condensation nuclei (CCN). Mass flux calculations suggest that short-lived convective cores (∼30 min) account for ∼2% of total vertical air mass transport relative to steady entrainment, increasing to ∼13% when the trailing stratiform regions are included. These results show that DC provides an episodic but efficient pathway linking the free troposphere and BL, influencing oxidant budgets, CCN variability, and climate forcing. Accurately representing this process in climate models may help reduce uncertainties in climate projections, under both preindustrial and present-day conditions.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Interseasonal Connections between the Timing of the Stratospheric Final Warming and Arctic Sea Ice

Connections across seasons in atmospheric circulation and sea ice have long been sought to advance seasonal prediction. This study presents a link between the springtime stratosphere and Arctic sea ice in summer through autumn. The polar stratospheric vortex dominates the winter stratosphere before breaking down each spring, which is called the stratospheric final warming, as solar radiation returns to the pole. Interannual variability of this breakdown is dynamically driven, leading to different springtime tropospheric and surface circulation patterns. To examine the different impacts of delayed and early final warmings, a multimodel composite was generated from selected CMIP5 models. Additionally, regressions were performed on JRA-55 against an index of springtime polar vortex strength. In both the multimodel composites and reanalysis regressions, significant anomalies in sea ice thickness persist several months following an anomalous timing of the final warming. A later final warming or stronger springtime polar stratospheric vortex leads to negative sea ice thickness anomalies in the East Siberian Sea and positive anomalies in the Beaufort Sea in comparison with an earlier final warming or weaker polar vortex. The spring polar stratospheric vortex is related to spring polar surface circulation patterns. The winds associated with this pattern induce anomalous sea ice motion, moving ice from the East Siberian Sea toward the Beaufort Sea. Reduced sea ice in the East Siberian Sea is linked to anomalous warmth over this region in autumn. Our results suggest that the timing of the stratospheric final warming exerts an influence on the tropospheric circulation and sea ice through autumn, which has implications for seasonal climate prediction.

Kelleher, Michael↗