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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 541 records · Page 30
All sourcesNASA NTRSDOE OSTI
DOE OSTI2016

Experimental particle formation rates spanning tropospheric sulfuric acid and ammonia abundances, ion production rates, and temperatures

Abstract Binary nucleation of sulfuric acid and water as well as ternary nucleation involving ammonia are thought to be the dominant processes responsible for new particle formation (NPF) in the cold temperatures of the middle and upper troposphere. Ions are also thought to be important for particle nucleation in these regions. However, global models presently lack experimentally measured NPF rates under controlled laboratory conditions and so at present must rely on theoretical or empirical parameterizations. Here with data obtained in the European Organization for Nuclear Research CLOUD (Cosmics Leaving OUtdoor Droplets) chamber, we present the first experimental survey of NPF rates spanning free tropospheric conditions. The conditions during nucleation cover a temperature range from 208 to 298 K, sulfuric acid concentrations between 5 × 10 5 and 1 × 10 9 cm −3 , and ammonia mixing ratios from zero added ammonia, i.e., nominally pure binary, to a maximum of ~1400 parts per trillion by volume (pptv). We performed nucleation studies under pure neutral conditions with zero ions being present in the chamber and at ionization rates of up to 75 ion pairs cm −3 s −1 to study neutral and ion‐induced nucleation. We found that the contribution from ion‐induced nucleation is small at temperatures between 208 and 248 K when ammonia is present at several pptv or higher. However, the presence of charges significantly enhances the nucleation rates, especially at 248 K with zero added ammonia, and for higher temperatures independent of NH 3 levels. We compare these experimental data with calculated cluster formation rates from the Atmospheric Cluster Dynamics Code with cluster evaporation rates obtained from quantum chemistry.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Rapid increase in tropospheric ozone over Southeast Asia attributed to changes in precursor emission source regions and sectors

Observations indicate that tropospheric ozone (O 3 ) concentrations over Southeast Asia have been increasing rapidly since the 1990s. Here, we quantify source contributions from geographical regions and emission sectors of the two distinct types of O 3 precursors, i.e., nitrogen oxides (NO x ) and volatile organic compounds (VOCs), to the increase in tropospheric O 3 in Southeast Asia during 1990–2019 using an O 3 source tagging technique implemented in a global chemistry-climate model. In this work, the results show that although local anthropogenic emission of NO x in Southeast Asia only contributes 18% of the annual averaged near-surface O 3 concentration, the increase in local NO x emission dominates the increasing trend of O 3 concentration in Southeast Asia, accounting for 107% of the regional averaged trend of 1.07 ppb decade -1 . Increases in NO x emissions from East Asia and South Asia explain 29% of the increasing trend, but 9% is offset by the emission reduction in North America. Ground transportation is responsible for 79% of the rapid O 3 increase, followed by 39% contribution from international shipping. Because an increase in anthropogenic NO x emissions enhances the O 3 production efficiency by VOCs, the increase in near-surface O 3 concentrations in Southeast Asia is thereby largely contributed by methane and biogenic VOCs.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Plant biochemistry influences tropospheric ozone formation, destruction, deposition, and response

Tropospheric ozone (O 3 ) is among the most damaging air pollutant to plants. Plants alter the atmospheric O 3 concentration in two distinct ways: (i) by the emission of volatile organic compounds (VOCs) that are precursors of O 3 ; and (ii) by dry deposition, which includes diffusion of O 3 into vegetation through stomata and destruction by nonstomatal pathways. Isoprene, monoterpenes, and higher terpenoids are emitted by plants in quantities that alter tropospheric O 3 . Deposition of O 3 into vegetation is related to stomatal conductance, leaf structural traits, and the detoxification capacity of the apoplast. The biochemical fate of O 3 once it enters leaves and reacts with aqueous surfaces is largely unknown, but new techniques for the tracking and identification of initial products have the potential to open the black box.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2022

Abundant Nitrate and Nitric Acid Aerosol in the Upper Troposphere and Lower Stratosphere

The tropospheric and stratospheric nitrate aerosol is simulated by a sectional aerosol model coupled to the Community Earth System Model. The simulated nitrate mass fractional contribution to aerosols is significantly higher in the upper troposphere and lower stratosphere (UTLS) than that at the surface. Both in situ measurements and simulations show that nitrate aerosol accounts for about 30%–40% of the aerosol mass at the tropopause of the Asian summer monsoon (ASM) region. Furthermore, simulated condensed nitric acid particles account for ~20% of the annual mean aerosol mass at the tropical tropopause, and over 95% in the UTLS at the South Pole in June-July-August. Here, our study suggests that the extremely cold ambient conditions in the UTLS of the tropics, ASM and polar regions thermodynamically favor the condensation of ammonia and nitric acid. The widely distributed nitrate aerosol in the global UTLS may be overlooked by climate models.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Recent Trends in Transport of Surface Carbonaceous Aerosols to the Upper-Troposphere-Lower-Stratosphere Linked to Expansion of the Asian Summer Monsoon Anticyclone

Using Modern-Era Retrospective analysis for Research and Applications Version-2 (MERRA-2) re-analyses, we have examined recent trends (2000–2019) in transport of surface carbonaceous aerosols (CAs), that is, organic carbon and black carbon, to the upper troposphere and lower stratosphere (UTLS) during the Asian summer monsoon (ASM). We find a significant increased concentration of UTLS CA, linked to a linear trend in an expansion of the Asian Summer Monsoon Anticyclone (ASMA). Over core monsoon latitudes (25°–35°N), the trends in UTLS CA are enabled by increased upward transport from surface sources via an intensified monsoon meridional circulation, with increased latent heating over the southern Tibetan Plateau and foothill regions, enhanced by feedback processes associated with radiative heating by UTLS CA. In the extra-tropics, increased UTLS CA stems primarily from an extended source of increased wildfire emissions over eastern Siberia and northern Asia, coincident with a large-scale anomalous anticyclone with enhanced surface warming and drying near (80°–120°E, 55°–70°N). Here, CAs are transported upward from the surface to the ULS, likely by increased pyro-convection associated with enhanced wildfires, and enter the tropical UTLS via increased equatorward transport on the eastern flanks of anomalous upper-level anticyclones, coupled to the expanded ASMA. Overall, the increasing UTLS CA trends associated with expansion of the ASMA are consistent with a hydrostatic expansion of a warming troposphere, reflected in a rise in the tropical tropopause and consequential dynamical adjustments of the ASM subtropical jetstream, modulating the climate of the greater ASM region.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2018

Photo-tautomerization of acetaldehyde as a photochemical source of formic acid in the troposphere

Organic acids play a key role in the troposphere, contributing to atmospheric aqueous-phase chemistry, aerosol formation, and precipitation acidity. Atmospheric models currently account for less than half the observed, globally averaged formic acid loading. Here we report that acetaldehyde photo-tautomerizes to vinyl alcohol under atmospherically relevant pressures of nitrogen, in the actinic wavelength range, λ = 300–330 nm, with measured quantum yields of 2–25%. Recent theoretical kinetics studies show hydroxyl-initiated oxidation of vinyl alcohol produces formic acid. Adding these pathways to an atmospheric chemistry box model (Master Chemical Mechanism) demonstrates increased formic acid concentrations by a factor of ~1.7 in the polluted troposphere and a factor of ~3 under pristine conditions. Incorporating this mechanism into the GEOS-Chem 3D global chemical transport model reveals an estimated 7% contribution to worldwide formic acid production, with up to 60% of the total modeled formic acid production over oceans arising from photo-tautomerization.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
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 OSTI2017

Tropospheric Warming Over The Past Two Decades

Satellite temperature measurements do not support the recent claim of a “leveling off of warming” over the past two decades. Tropospheric warming trends over recent 20-year periods are always significantly larger (at the 10% level or better) than model estimates of 20-year trends arising from natural internal variability. Over the full 38-year period of the satellite record, the separation between observed warming and internal variability estimates is even clearer. In two out of three recent satellite datasets, the tropospheric warming from 1979 to 2016 is unprecedented relative to internally generated temperature trends on the 38-year timescale.

54 ENVIRONMENTAL SCIENCES↗
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 OSTI2015

Active and widespread halogen chemistry in the tropical and subtropical free troposphere

Significance Our measurements show that tropospheric halogen chemistry has a larger capacity to destroy O 3 and oxidize atmospheric mercury than previously recognized. Halogen chemistry is currently missing in most global and climate models, and is effective at removing O 3 at altitudes where intercontinental O 3 transport occurs. It further helps explain the low O 3 levels in preindustrial times. Public health concerns arise from bioaccumulation of the neurotoxin mercury in fish. Our results emphasize that bromine chemistry in the free troposphere oxidizes mercury at a faster rate, and makes water-soluble mercury available for scavenging by thunderstorms. Naturally occurring bromine in air aloft illustrates global interconnectedness between energy choices affecting mercury emissions in developing nations and mercury deposition in, e.g., Nevada, or the southeastern United States.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Mean precipitation change from a deepening troposphere

Global climate models robustly predict that global mean precipitation should increase at roughly 2–3% K - 1 , but the origin of these values is not well understood. Here we develop a simple theory to help explain these values. This theory combines the well-known radiative constraint on precipitation, which says that condensation heating from precipitation is balanced by the net radiative cooling of the free troposphere, with an invariance of radiative cooling profiles when expressed in temperature coordinates. These two constraints yield a picture in which mean precipitation is controlled primarily by the depth of the troposphere, when measured in temperature coordinates. We develop this theory in idealized simulations of radiative–convective equilibrium and also demonstrate its applicability to global climate models.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2018

Rapid growth of organic aerosol nanoparticles over a wide tropospheric temperature range

Nucleation and growth of aerosol particles from atmospheric vapors constitutes a major source of global cloud condensation nuclei (CCN). The fraction of newly formed particles that reaches CCN sizes is highly sensitive to particle growth rates, especially for particle sizes <10 nm, where coagulation losses to larger aerosol particles are greatest. Currnet results show that some oxidation products from biogenic volatile organic compounds are major contributors to particle formation and initial growth. However, whether oxidized organics contribute to particle growth over the broad span of tropospheric temperatures remains an open question, and quantitative mass balance for organic growth has yet to be demonstrated at any temperature. Here, in experiments performed under atmospheric conditions in the Cosmics Leaving Outdoor Droplets (CLOUD) chamber at the European Organization for Nuclear Research (CERN), we show that rapid growth of organic particles occurs over the range from – 25 ° C to 25 ° C. The lower extent of autoxidation at reduced temperatures is compensated by the decreased volatility of all oxidized molecules. This is confirmed by particle-phase composition measurements, showing enhanced uptake of relatively less oxygenated products at cold temperatures. We can reproduce the measured growth rates using an aerosol growth model based entirely on the experimentally measured gas-phase spectra of oxidized organic molecules obtained from two complementary mass spectrometers. We report that the growth rates are sensitive to particle curvature, explaining widespread atmospheric observations that particle growth rates increase in the single-digit-nanometer size range. Our results demonstrate that organic vapors can contribute to particle growth over a wide range of tropospheric temperatures from molecular cluster sizes onward.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Internal variability and forcing influence model–satellite differences in the rate of tropical tropospheric warming

Climate-model simulations exhibit approximately two times more tropical tropospheric warming than satellite observations since 1979. The causes of this difference are not fully understood and are poorly quantified. Here, we apply machine learning to relate the patterns of surface-temperature change to the forced and unforced components of tropical tropospheric warming. This approach allows us to disentangle the forced and unforced change in the model-simulated temperature of the midtroposphere (TMT). In applying the climate-model-trained machine-learning framework to observations, we estimate that external forcing has produced a tropical TMT trend of 0.25 ± 0.08 K⋅decade −1 between 1979 and 2014, but internal variability has offset this warming by 0.07 ± 0.07 K⋅decade −1 . Using the Community Earth System Model version 2 (CESM2) large ensemble, we also find that a discontinuity in the variability of prescribed biomass-burning aerosol emissions artificially enhances simulated tropical TMT change by 0.04 K⋅decade −1 . The magnitude of this aerosol-forcing bias will vary across climate models, but since the latest generation of climate models all use the same emissions dataset, the bias may systematically enhance climate-model trends over the satellite era. Our results indicate that internal variability and forcing uncertainties largely explain differences in satellite-versus-model warming and are important considerations when evaluating climate models.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2016

Satellite Sounder Observations of Contrasting Tropospheric Moisture Transport Regimes: Saharan Air Layers, Hadley Cells, and Atmospheric Rivers

This paper examines the performance of satellite sounder atmospheric vertical moisture proles (AVMP) under tropospheric conditions encompassing moisture contrasts driven by convection and advection transport mechanisms, specifically Atlantic Ocean Saharan air layers (SALs) and Pacific Ocean moisture conveyer belts (MCBs) commonly referred to as atmospheric rivers (ARs), both of these being mesoscale to synoptic meteorological phenomena within the vicinity of subtropical Hadley subsidence zones. Operational AVMP environmental data records retrieved from the Suomi National Polar-orbiting Partnership (SNPP) NOAA-Unique Combined Atmospheric Processing System (NUCAPS) are collocated with dedicated radiosonde observations (RAOBs) obtained from ocean-based intensive field campaigns; these RAOBs provide uniquely independent correlative truth data not assimilated into numerical weather prediction models for satellite sounder validation over open ocean. Using these marine-based data, we empirically assess the performance of the operational NUCAPS AVMP product for detecting and resolving these tropospheric moisture features over otherwise RAOB-sparse regions.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Afterpulse correction for micro-pulse lidar to improve middle and upper tropospheric aerosol measurements

Micro-pulse lidar (MPL) measurements have been widely used in atmospheric research over the past few decades. However, the MPL afterpulse noise has a large impact on the MPL aerosol measurement in the middle and upper troposphere, and an effective correction method is still lacking. Here, a new afterpulse correction approach is presented by using measurements with low-level optically thick clouds to act as the lids blocking atmospheric signals beyond the clouds completely. Examples are provided to illustrate the effectiveness of this correction method. Using one-year 2014 MPL measurements at the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) North Slope of Alaska (NSA) site, the impact of the correction on the aerosol measurements is quantified. The relative error (RE, %) of attenuated backscattering ratio (ABR) without the afterpulse correction is 30% and 190% at the height of 1.00 km and 9.00 km (AGL), and the RE is larger for weaker aerosol signals (ABR<2). The RE of linear depolarization ratio (LDR), which is significantly higher than that of ABR for a given aerosol layer, is highly non-linear above 3.00 km, with a value of 300%-900% for weak aerosols (ABR<2) above 3.00 km. Therefore, the afterpulse correction is critical for the middle and upper tropospheric aerosol observations. We demonstrated that our afterpulse correction can provide reasonable particle depolarization ratio (PDR) to properly identify dust aerosols. The newly developed method can be applied to long-term MPL measurements to support aerosol and mixed-phase/ice cloud interaction study at the NSA site.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Beryllium Isotopes in Rainfall for Stratospheric-Tropospheric Exchange Dynamics Experiment (BIRDIE) (Final Report)

The Beryllium Isotopes in Rainfall for Stratospheric-Tropospheric Exchange Dynamics Experiment or BIRDIE was a precipitation collection campaign designed to measure cosmogenic isotopes of beryllium in rainfall and other forms of precipitation across the DOE Southern Great Plains (SGP) Atmospheric Radiation Measurement (ARM) site. Precipitation samples were collected over three weeks (May 21-June 10, 2022) at 11 SGP sites across a 120 km 2 domain in northern and central Oklahoma. The field campaign targeted summer-time convection rain events. We aimed to capture any spatial and/or temporal variability in the concentrations of beryllium-10 (10Be) and beryllium-7 (7Be) across the SGP ARM site during these rainfall events. The ratio of 10Be to 7Be (10/7Be) has been shown to be a powerful tracer for transport processes in the stratosphere-troposphere exchange (STE) system (e.g., Koch and Rind 1998). Any observed variability is analyzed to see if it could be linked to STE processes, including overshooting of deep convection clouds which penetrate the lower stratosphere. Six wet weather system events were collected within our three-week span. Five out of six of these rainfall events are classified as moderately to strongly convective. Those events are studied in more detail. The five systems also follow each other over a short time period of eleven days. In our rainfall samples we observed spatial and event variability in the concentrations of beryllium-10 and -7 which resulted in variability of 10/7 Be ratios. Each weather event appeared to exhibit a unique 10/7Be pattern across the domain that was not directly linked to storm total precipitation amount. To better understand the causes for this spatial variability, cloud characteristics in the domain were looked at to assess cloud type, cloud height and depth information. We also ran Hysplit back trajectories to identify possible air mass and moisture origins across our events. Detailed analysis is still on-going. The purpose of this technical report is to provide background on using cosmogenic isotopes as atmospheric tracers, describe the experimental design, and present the beryllium concentration and ratio data.

58 GEOSCIENCES↗
DOE OSTI2023

Beryllium Isotopes in Rainfall for Stratospheric-Tropospheric Exchange Dynamics Experiment (BIRDIE) (Field Campaign Report)

The Beryllium Isotopes in Rainfall for Stratospheric-Tropospheric Exchange Dynamics Experiment or BIRDIE was a precipitation collection campaign designed to measure cosmogenic isotopes of beryllium in rainfall and other forms of precipitation across the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility’s Southern Great Plains (SGP) atmospheric observatory. Precipitation samples were collected over three weeks (May 21-June 10, 2022) at 11 SGP sites across a 120-km 2 domain in northern and central Oklahoma. The field campaign targeted summertime convection rain events. We aimed to capture any spatial and/or temporal variability in the concentrations of beryllium-10 (10Be) and beryllium-7 (7Be) across the ARM SGP site during these rainfall events. The ratio of 10Be to 7Be (10/7Be) has been shown to be a powerful tracer for transport processes in the stratosphere-troposphere exchange (STE) system (e.g., Koch and Rind 1998). Any observed variability is analyzed to see if it could be linked to STE processes, including overshooting of deep convection clouds that penetrate the lower stratosphere. Six wet weather system events were collected within our three-week span. Five out of six of these rainfall events are classified as moderately to strongly convective. Those events are studied in more detail. The five systems also follow each other over a short period of 11 days. In our rainfall samples we observed spatial and event variability in the concentrations of beryllium-10 and -7 that resulted in variability of 10/7Be ratios. Each weather event appeared to exhibit a unique 10/7Be pattern across the domain that was not directly linked to storm total precipitation amount. To better understand the causes for this spatial variability, cloud characteristics in the domain were looked at to assess cloud type, cloud height, and depth information. We also ran Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model back trajectories to identify possible air mass and moisture origins across our events. Detailed analysis is ongoing. The purpose of this technical report is to provide background on using cosmogenic isotopes as atmospheric tracers, describe the experimental design, and present the beryllium concentration and ratio data. Lastly, we note that BIRDIE coincided with two other deep convection field campaigns in the area: The National Aeronautics and Space Administration (NASA)’s Dynamics and Chemistry of the Summer Stratosphere (DCOTSS) experiment (https://dcotss.org/) centered in Salina, Kansas, and the Targeted Observation by Radars and (uncrewed aerial systems) UAS of Supercells (TORUS) experiment (https://catalog.eol.ucar.edu/torus_2022) across the U.S. Central Plains. Additionally, a Lawrence Livermore National Laboratory ( LLNL) team at DCOTSS attempted to measure 10Be/7Be ratios on aerosols collected in situ in the lower and mid-stratosphere over Kansas using high-altitude balloons. Precipitation samples were also collected on the ground in Salina, Kansas.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2017

Lower-tropospheric CO 2 from near-infrared ACOS-GOSAT observations

We present two new products from near-infrared Greenhouse Gases Observing Satellite (GOSAT) observations: lowermost tropospheric (LMT, from 0 to 2.5 km) and upper tropospheric–stratospheric ( U , above 2.5 km) carbon dioxide partial column mixing ratios. We compare these new products to aircraft profiles and remote surface flask measurements and find that the seasonal and year-to-year variations in the new partial column mixing ratios significantly improve upon the Atmospheric CO 2 Observations from Space (ACOS) and GOSAT (ACOS-GOSAT) initial guess and/or a priori, with distinct patterns in the LMT and U seasonal cycles that match validation data. For land monthly averages, we find errors of 1.9, 0.7, and 0.8 ppm for retrieved GOSAT LMT, U , and X CO 2 ; for ocean monthly averages, we find errors of 0.7, 0.5, and 0.5 ppm for retrieved GOSAT LMT, U , and X CO 2 . In the southern hemispheric biomass burning season, the new partial columns show similar patterns to MODIS fire maps and MOPITT multispectral CO for both vertical levels, despite a flat ACOS-GOSAT prior, and a CO–CO 2 emission factor comparable to published values. The difference of LMT and U , useful for evaluation of model transport error, has also been validated with a monthly average error of 0.8 (1.4) ppm for ocean (land). LMT is more locally influenced than U , meaning that local fluxes can now be better separated from CO 2 transported from far away.

54 ENVIRONMENTAL SCIENCES↗