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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 73 records · Page 4
All sourcesNASA NTRSDOE OSTI
NASA NTRS2013

Impacts of Climate Change on Surface Ozone and Intercontinental Ozone Pollution: A Multi-Model Study

The impact of climate change between 2000 and 2095 SRES A2 climates on surface ozone (O)3 and on O3 source-receptor (S-R) relationships is quantified using three coupled climate-chemistry models (CCMs). The CCMs exhibit considerable variability in the spatial extent and location of surface O3 increases that occur within parts of high NOx emission source regions (up to 6 ppbv in the annual average and up to 14 ppbv in the season of maximum O3). In these source regions, all three CCMs show a positive relationship between surface O3 change and temperature change. Sensitivity simulations show that a combination of three individual chemical processes-(i) enhanced PAN decomposition, (ii) higher water vapor concentrations, and (iii) enhanced isoprene emission-largely reproduces the global spatial pattern of annual-mean surface O3 response due to climate change (R2 = 0.52). Changes in climate are found to exert a stronger control on the annual-mean surface O3 response through changes in climate-sensitive O3 chemistry than through changes in transport as evaluated from idealized CO-like tracer concentrations. All three CCMs exhibit a similar spatial pattern of annual-mean surface O3 change to 20% regional O3 precursor emission reductions under future climate compared to the same emission reductions applied under present-day climate. The surface O3 response to emission reductions is larger over the source region and smaller downwind in the future than under present-day conditions. All three CCMs show areas within Europe where regional emission reductions larger than 20% are required to compensate climate change impacts on annual-mean surface O3.

Troposphere: constituent transport and chemistry↗
NASA NTRS2017

An Overview of Atmospheric Chemistry and Air Quality Modeling

This presentation will include my personal research experience and an overview of atmospheric chemistry and air quality modeling to the participants of the NASA Student Airborne Research Program (SARP 2017). The presentation will also provide examples on ways to apply airborne observations for chemical transport (CTM) and air quality (AQ) model evaluation. CTM and AQ models are important tools in understanding tropospheric-stratospheric composition, atmospheric chemistry processes, meteorology, and air quality. This presentation will focus on how NASA scientist currently apply CTM and AQ models to better understand these topics. Finally, the importance of airborne observation in evaluating these topics and how in situ and remote sensing observations can be used to evaluate and improve CTM and AQ model predictions will be highlighted.

Atmospheric↗
NASA NTRS2020

Sensitivity of Tropospheric Ozone Over the Southeast USA to Dry Deposition

Dry deposition (DD) is a major loss process for tropospheric ozone and some reactive nitrogen and carbon precursors. We investigate the response of summertime ozone and its production chemistry over the Southeast United States (USA) to variability in this sink. Turning off DD of oxidized nitrogen, ozone, or all species over the United States in the Geophysical Fluid Dynamics Laboratory AM3 model increases regional mean surface ozone by 5, 18, or 25 ppb, respectively. Additional sensitivity simulations demonstrate that, assuming linearity, surface ozone has a similar sensitivity to ozone DD as to NOx emissions. Trends in ozone production efficiency derived from observed relationships between ozone and precursor oxidation products may not solely reflect precursor emission changes if ozone DD varies (e.g., with meteorology). We conclude that DD variability merits consideration when interpreting observed ozone trends. Quantifying the impact of changes in sinks versus sources will require long‐term DD measurements across the region of interest.

dry deposition↗
NASA NTRSDate not supplied

Sub-Seasonal Variability of the Asian Summer Monsoon Transport of CO and Aerosols to the UTLS and Implications for Global Atmospheric Composition

The upper troposphere/ lower stratosphere (UTLS) is a climate sensitive region. The Asian summer monsoon (ASM) is a major component in the climate system. It transports aerosols and trace gases from the most polluted regions in Asia to UTLS where they spread out to the global atmosphere. Although ASM is a seasonal phenomenon with strongest global influences usually seen in summer, it is highly dynamic and connected to other weather and climate systems, with significant spatial and temporal variability ranging from sub-seasonal weather scale to multi-year climate scale. The interplay of multi-scale dynamics inevitably determines the variability of the transport pathways and atmospheric composition in the UTLS.

sub-seasonal variability↗
NASA NTRS1999

Biomass Burning Influences on the Composition of the Remote South Pacific Troposphere: Analysis Based on Observations from PEM Tropics-A

Airborne, in-situ measurements from PEM-Tropics-A (September/October 1996) are analyzed to show the presence of distinct pollution plumes in the middle-tropical troposphere of the remote South Pacific (10-30degS). These elevated plumes cause a relative maximum at about 5-7km attitude in the vertical distribution of primary and secondary species characteristic of fuel combustion and biomass burning (CO, C2H2, C2H6, CH3Cl, PAN, O3). Similar plumes were also observed at mid-latitudes in the middle troposphere during three flights east of New Zealand (40-45degS). In all, pollution plumes with CO larger than 100 ppb were observed 24 times on 7 separate flight days south of the equator. The observed plumes were generally embedded in very dry air. Ten-day back trajectory analysis supports the view that these originated from the biomass burning regions of South Africa (and South America) and were transported to the South Pacific along long-distance subsiding trajectories. The chemical composition of the southern Pacific troposphere analyzed from the PEM-Tropics-A data is compared with data from the tropical regions of the northern Pacific (PEM-West-A) and southern Atlantic (TRACE-A) during the same Sept/Oct time period. Sizable perturbations in the abundance of ozone and its key precursors, resulting from the transport of pollution originating from biomass burning sources, are observed in much of the Southern Hemispheric troposphere.

Singh, H. B.↗
NASA NTRS1989

Amazon capims (floating grassmats) - A source of C-13 enriched methane to the troposphere

The C-13 isotopic composition of methane emitted to the troposphere from Amazon capims (floating grassmats) ranged from -36.9 to -48.0, per mil averaging -44.4 + or - 4.2 per mil. All pools of methane associated with the grassmats were enriched; methane withdrawn from plant stems ranged from -39 to -49 per mil while bubbles stirred from the root mat averaged -41.4 per mil. As the CH4 flux from these habitats makes up some 40 percent of the total flux from the Amazon floodplain, methane emissions from the region as a whole must be enriched in.

Chanton, Jeffrey↗
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↗
NASA NTRS1994

Low to middle tropospheric profiles and biosphere/troposphere fluxes of acidic gases in the summertime Canadian taiga

We report features of acidic gases in the troposphere from 9 to 5000 m altitude above ground over the Canadian taiga in the summer of 1990. The measurements were conducted at a 30-m meteorological tower and from the NASA Wallops Electra aircraft as part of the joint U.S.-Canadian Arctic Boundary Layer Expedition (ABLE) 3B Northern Wetland Studies (NOWES). We sampled air for acidic gases using the mist chamber collector coupled with subsequent analysis using ion chromatography. At the tower we collected samples at two heights during a 13-day period, including diurnal studies. Using eddy flux and profile data, we estimated the biosphere/troposphere fluxes of nitric, formic, and acetic acids and sulfur dioxide. For the organic acids, emissions from the taiga in the afternoon hours and deposition during the predawn morning hours were observed. The flux intensities alone were however not high enough to explain the observed changes in mixing ratios. The measured deposition fluxes of nitric acid were high enough to have a significant influence on its mixing ratio in the boundary layer. On three days we measured vertical profiles of nitric, formic, and acetic acids through the lower to midtroposphere. We found that the chemical composition of the troposphere was extremely heterogenous. Pronounced layers of polluted air were readily apparent from our measurements. Local photochemical production and episodic long-range transport of trace components, originating from biomass burning and possibly industrial emissions, appear to have a strong influence on the composition of the troposphere and biosphere/troposphere fluxes of acidic gases at this site.

Klemm, O.↗
NASA NTRS2019

Emissions Relationships in Western Forest Fire Plumes: I. Reducing the Effect of Mixing Errors on Emission Factors

Studies of emission factors from biomass burning using aircraft data complement the results of lab studies and extend them to conditions of immense hot conflagrations. We illustrate and discuss emission relationships for 422 individual samples from many forest-fire plumes in the Western US. The samples are from two NASA investigations: ARCTAS (Arctic Research of the Composition of the Troposphere from Aircraft and Satellites) and SEAC4RS (Studies of Emissions and Atmospheric Composition, Clouds, and Climate Coupling by Regional Surveys). This work provides sample-by-sample enhancement ratios (EnRs) for 23 gases and particulate properties. Many EnRs provide candidates for emission ratios (ERs, corresponding to the EnR at the source) when the origin and degree of transformation is understood and appropriate. From these, emission factors (EFs) can be estimated when the fuel dry mass consumed is known or can be estimated using the carbon mass budget approach. This analysis requires understanding the interplay of mixing of the plume with surrounding air. Some initial examples emphasize that measured C(tot) = CO2 + CO in a fire plume does not necessarily describe the emissions of the total carbon liberated in the flames, C(burn). Rather, it represents C(tot) = C(burn) + C(bkgd), which includes possibly varying background concentrations for entrained air. Consequently, we present a simple theoretical description for plume entrainment for multiple tracers from flame to hundreds of kilometers downwind and illustrate some intrinsic linear behaviors. The analysis suggests a Mixed Effects Regression Emission Technique (MERET), which can eliminate occasional strong biases associated with the commonly used normalized excess mixing ratio (NEMR) method. MERET splits C(tot) to reveal C(burn) by exploiting the fact that C(burn) and all tracers respond linearly to dilution, while each tracer has consistent EnR behavior (slope of tracer concentration with respect to C(burn)). The two effects are separable. Two or three or preferably more emission indicators are required as a minimum; here we used ten. Limited variations in the EnRs for each tracer can be incorporated and the variations and co-variations analyzed. The percentage CO yield (or the modified combustion efficiency) plays some role. Other co-relationships involving nitrogen and organic classes are more prominent; these have strong relationships to the C(burn) to O3 emission relationship. In summary, MERET allows fine spatial resolution (EnRs for individual observations) and comparison of similar plumes distant in time and space. Alkene ratios provide us with an approximate photochemical timescale. This allows discrimination and definition, by fire situation, of ERs, allowing us to estimate emission factors.

Chatfield, Robert B.↗
NASA NTRS1998

Combining data from lidar and in situ instruments to characterize the vertical structure of aerosol optical properties

Over the last decade, the quantification of tropospheric aerosol abundance, composition and radiative impacts has become an important research endeavor. For the most part, the interest in tropospheric aerosols is derived from questions related to the global and local (instantaneous) radiative forcing of climate due to these aerosols. One approach is to study local forcing under well-defined conditions, and to extrapolate such results to global scales. To estimate local aerosol forcing, appropriate radiative transfer models can be employed (e.g., the Fu-Liou radiative transfer code, [Fu and Liou, 1993]). In general, such models require information on derived aerosol properties [Toon, 1994]; namely the aerosol optical depth, single-scattering albedo, and asymmetry factor (phase function), all of which appear in the equations of radiative transfer. In this paper, we report on a method that utilizes lidar data and in situ aerosol size distribution measurements to deduce the vertical structure of the aerosol complex index of refraction in the near IR, thus identifying the aerosol type. Together with aerosol size distributions obtained in situ, the aerosol refractive index can be used to calculate the necessary derived aerosol properties. The data analyzed here were collected during NASA's PEM West-B (Pacific Exploratory Mission) experiment, which took place in February/March 1994. The platform for the measurements was the NASA DC-8 aircraft. The primary goal of the PEM West missions [Browell et al., 1996] was the assessment of potential anthropogenic perturbations of the chemistry in the Pacific Basin troposphere. For this purpose the timing of PEM West-B corresponded to the seasonal peak in transport from the Asian continent into the Pacific basin [Merrill et al., in press]. This period normally occurs during Northern Hemisphere spring, when the Japan jet is well developed.

Redemann, J.↗
NASA NTRS1985

Influence of meteorological conditions on aerosol vertical distribution and composition off the northeast American coastline

The size distribution and composition of lower tropospheric aerosols were measured off the northeast American coastline under clear air and disturbed meteorological conditions. Under the clear air conditions observed on 5 August 1982, with air flow from west to east, sulfate-rich stratified layers are the dominant feature of aerosol distribution in the lowest 3000 m of the troposphere. The encroachment of a warm frontal system over the study area on 9 August 1982 resulted in dramatic changes in aerosol distribution and composition prior to any precipitation, probably due to increased vertical mixing and dilution of pollutant aerosols. Chloride becomes the dominant water soluble anion in the lower 3000 m, primarily due to a several fold decrease in sulfate. Although these results are limited to only two sets of measurements, the data indicate the variability which can occur in the tropospheric vertical aerosol distributions at remote locations. A knowledge of the structure and stability of these stratified layers is of particular importance to studies of the ocean-troposphere chemistry problem.

Sebacher, D. I.↗
NASA NTRS1994

Chemical composition of the atmospheric aerosol in the troposphere over the Hudson Bay lowlands and Quebec-Labrador regions of Canada

Atmospheric aerosols were collected in the boundary layer and free troposphere over continental and coastal subarctic regions of Canada during the July - August 1990 joint U.S.-Canadian Arctic Boundary Layer Expedition (ABLE) 3B/Northern Wetlands Study (NOWES). The samples were analyzed for the following water soluble species: sulfate, nitrate, ammonium, potassium, sodium, chloride, oxalate, methylsulfonate, and total amine nitrogen. Ammonium and sulfate were the major water soluble components of these aerosols. The nearly neutral (overall) chemical composition of summertime aerosol particles contrasts their strongly acidic wintertime composition. Aerosol samples were separated into several air mass categories and characterized in terms of chemical composition, associated mixing ratios of gaseous compounds, and meteorological parameters. The fundamental category represented particles associated with 'background' air masses. The summertime atmospheric aerosols in background air over the North American subarctic and Arctic regions were characterized by relatively small and spatially uniform mixing ratios of the measured species. These aerosol particles were aged to the extent that they had lost their primary source signature. The chemical profile of the background air aerosols was frequently modified by additions from biomass fire plumes, aged tropical marine air, and intrusions of upper tropospheric/lower stratospheric air. Aerosols in boundary layer background air over the boreal forest region of Quebec-Labrador had significantly larger mixing ratios of ammonium and sulfate relative to the Hudson Bay region. This may reflect infiltration of anthropogenic pollution or be due to natural emissions from this region.

Gorzelska, K.↗
NASA NTRS2001

Satellite Observations of Tropospheric Chemistry

The troposphere is an essential component of the earth's life support system as well as the gateway for the exchange of chemicals between different geochemical reservoirs of the earth. The chemistry of the troposphere is sensitive to perturbation from a wide range of natural phenomena and human activities. The societal concern has been greatly enhanced in recent decades due to ever increasing pressures of population growth and industrialization. Chemical changes within the troposphere control a vast array of processes that impact human health, the biosphere, and climate. A main goal of tropospheric chemistry research is to measure and understand the response of atmospheric composition to natural and anthropogenic perturbations, and to develop the capability to predict future change. Atmospheric chemistry measurements are extremely challenging due to the low concentrations of critical species and the vast scales over which the observations must be made. Available tropospheric data are mainly from surface sites and aircraft missions. Because of the limited temporal extent of aircraft observations, we have very limited information on tropospheric composition above the surface. This situation can be contrasted to the stratosphere, where satellites have provided critical and detailed chemical data on the global distribution of key trace gases.

Singh, Hanwant B.↗
NASA NTRS2021

Intercomparison of the representations of the atmospheric chemistry of pre-industrial methane and ozone in earth system and other global chemistry-transport models

An intercomparison has been set up to study the representation of the atmospheric chemistry of the pre-industrial troposphere in earth system and other global tropospheric chemistry-transport models. The intercomparison employed a constrained box model and utilised tropospheric trace gas composition data for the pre-industrial times at ninety mid-latitude surface locations. Incremental additions of four organic compounds: methane, ethane, acetone and propane, were used to perturb the constrained box model and generate responses in hydroxyl radicals and tropospheric ozone at each location and with each chemical mechanism. Although the responses agreed well across the chemical mechanisms from the selected earth system and other global tropospheric chemistry-transport models, there were differences in the detailed responses between the chemical mechanisms that could be tracked down by sensitivity analysis to differences in the representation of C1–C3 chemistry. Inter-mechanism ranges in NOx compensation points were about 0.17 ± 0.12 when expressed relative to the inter-mechanism average. Monte Carlo uncertainty analysis carried out with a single chemical mechanism put the intra-mechanism range a factor of three higher at 0.50 ± 0.12. Similar differences between inter-mechanism and intra-mechanism ranges were found for hydroxyl radical depletion but were up to a factor of six wider for ozone formation from incremental additions of organic compounds. The cause of the discrepancies between the inter- and intra-mechanism ranges was found to be the large uncertainties that are present in the laboratory determinations of the rate coefficients and product channel branching ratios of some key chemical reactions involving organic peroxy radicals and hydroperoxides. Whilst these large uncertainties are present in the laboratory determinations, there will be irreducible uncertainties in the predictions from the earth system and other chemistry-transport models of methane and tropospheric ozone trends since pre-industrial times and hence their contributions to the radiative forcing of climate change. Further definitive laboratory studies of the reaction rates and product yields of the reactions of the simple organic peroxy radicals and hydroperoxides are required to resolve and reduce current uncertainties in earth system and chemistry-transport model predictions.

atmospheric chemistry↗
NASA NTRS1987

The role of aqueous chemistry in determining the composition and cloud structure of the upper troposphere on Uranus

Aqueous chemistry on Uranus affects the atmospheric abundances of NH3 and H2S below the methane cloud base. Here a complete thermochemical equilibrium model for the H2O-NH3-H2S system is presented. Inclusion of H2S increases the aqueous removal of NH3 to 20-30 percent, but aqueous chemistry alone cannot account for the depletion of NH3 in the 150-200-K region of the atmosphere required to fit microwave observations. Formation of NH4SH clouds can account for the observed depletion provided the H2S/NH3 ratio is enhanced by a factor of 4 relative to solar. Perturbations to the chemical balance between N and S, for example by the general circulation on Uranus, would then produce regions with either NH3 or H2S aloft.

Carlson, Barbara E.↗
NASA NTRS2005

Gases and Aerosols over North America and the Atlantic: First results from INTEX-A

Intercontinental Chemical Transport Experiment (INTEX; http://cloud1.arc.nasa.gov) is an ongoing two-phase integrated atmospheric field experiment being performed over North America (NA). Its first phase (INTEX-A) was performed in the summer of 2004 and the second phase (INTEX-B) is planned for the early spring of 2006. The main goal is to characterize the sources and distribution of gases and aerosols over NA and to understand their transport and transformation on transcontinental/intercontinental scales in order to assess their impact on air quality and climate. Central to achieving this goal is the need to relate space-based observations with those from airborne and surface platforms. During JNTEX-A, NASA s DC-8 was joined by some dozen other aircraft from a large number of European (U. K., France, and Germany) and North American partners to explore the composition of the troposphere over NA and the Atlantic in a coordinated manner. Global and regional models along with satellite observations were extensively used to plan, coordinate, and implement this field mission. Aircraft were instrumented to measure a comprehensive suite of gases and aerosols utilizing in-situ and remote sensors. The NASA DC-8 alone was equipped with some 20 instruments capable of measuring species at concentrations as low as 10(exp -15) v/v. Measurements included major atmospheric gaseous constituents (O3, NO(x), HNO3, HNO4, PANS, SO2, VOC/OVOC, CO, and CO2), free radicals and precursors (OH, HO2, H2O2, HCHO), aerosols and radiation (microphysics, composition, optical depth, radiative flux), as well as multiple tracers of pollution. Validation of instruments aboard Terra, Aqua, and Envisat satellites was given high priority. Some of the highest pollution levels were present in the upper troposphere due to widespread deep convection. Although unexpected, frequent instances of Asian pollution over NA were encountered during these summer months. The soil uptake of CO2 over NA was characterized over large regions of NA helping to understand the continents CO2-sink potential. DC-8 sampling of smoke from Alaskan fires and formaldehyde over forested regions, and simultaneous satellite observations of these provided excellent opportunities for the interplay of these platforms. Outflow of pollution from NA was sampled again over the Atlantic after several days to assess its evolution during transport. Models of chemistry and radiation are presently being employed to help in the interpretation of JNTEX-A data. The planning for INTEX-B (spring 2006) is currently underway. First results from INTEX-A and plans for INTEX-B will be discussed

Singh, Hanwant B.↗
NASA NTRS1976

Atmospheric ozone measurements made from B-747 airliners - Spring 1975

Atmospheric ozone in the upper troposphere and lower stratosphere north of the equator has been registered aboard two commercial B-747 airliners during the Spring of 1975. This monitoring is part of a much broader and continuing project developed by NASA and known as the Global Atmospheric Sampling Program (GASP). Additional flight and meteorological conditions have also been automatically recorded on board concurrent with the ozone measurements. Independently-derived tropopause pressure information was available from NMC data archives and was used to identify stratospheric and tropospheric flight. The composite ozone, flight and meteorological data are reported for selected dates in March, April, and May. Attention is drawn particularly to the vertical profiles of atmospheric ozone mixing ratio as a function of both distance from the tropopause and curvature of the streamlines. The GASP observations suggest that ozone levels typical of the lower stratosphere are often embedded in the upper troposphere, principally during occasions when cyclonic wind curvature was noted.

Falconer, P. D.↗