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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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NASA NTRS1982

Clouds and wet removal as causes of variability in the trace-gas composition of the marine troposphere

A modeling study of the effects of clouds and wet removal on the chemistry of the remote marine troposphere is described. Using a time-dependent model with parameterized vertical transport to calculate trace-gas concentrations, it is found that large variations in key species (e.g., HNO3, H2CO, and H2O2) result from simulations of sporadic rainfall, changes in cloud cover, and external inputs such as surface NO sources. Depending on the frequency and intensity of an event, the effects of these perturbations may persist for several days, thereby invalidating assumptions of photochemical equilibrium in the interpretation of measurements. Long-term integrations with fixed boundary conditions and regularly occurring cloud and rain episodes demonstrate a strong sensitivity of the mean concentration of longer-lived soluble gases to precipitation frequency but also confirm the validity of using properly chosen parameterizations of wet removal in steady state calculations.

Thompson, A. M.↗
NASA NTRS2005

Atmospheric Hydroperoxides in West Antarctica: Links to Stratospheric Ozone and Atmospheric Oxidation Capacity

The troposphere above the West Antarctic Ice Sheet (WAIS) was sampled for hydroperoxides at 21 locations during 2-month-long summer traverses from 2000 to 2002, as part of US ITASE (International Transantarctic Scientific Expedition). First time quantitative measurements using an HPLC method showed that methylhydroperoxide (MHP) is the only important organic hydroperoxide occurring in the Antarctic troposphere, and that it is found at levels ten times those previously predicted by photochemical models. During three field seasons, means and standard deviations for hydrogen peroxide (H2O2) were 321+/-158 pptv, 650+/-176 pptv and 330+/-147 pptv. While MHP was detected, but not quantified in December 2000, levels in summer 2001 and 2002 were 317+128 pptv and 304+/-172.2 pptv. Results from firn air experiments and diurnal variability of the two species showed that atmospheric H2O2 is significantly impacted by a physical snow pack source between 76 and 90degS, whereas MHP is not. We show strong evidence of a positive feedback between stratospheric ozone and H2O2 at the surface. Between November-27 and December-12 in 2001, when ozone column densities dropped below 220 DU (means in 2000 and 2001 were 318 DU and 334 DU, respectively), H2O2 was 1.7 times that observed in the same period in 2000 and 2002, while MHP was only 80% of the levels encountered in 2002. Photochemical box model runs suggest that NO and OH levels on WAIS are closer to coastal values, while Antarctic Plateau levels are higher, confirming that region to be a highly oxidizing environment. The modeled sensitivity of H2O2 and particularly MHP to NO offers the potential to use atmospheric hydroperoxides to constrain the NO background and thus estimate the past oxidation capacity of the remote atmosphere. Index Terms: 0365 Atmospheric Composition and Structure: Troposphere: composition and chemistry; 0322 Atmospheric Composition and Structure: Constituent sources and sinks; 1610 Global Change: Atmosphere (03 15,0325); 0736 Cryosphere: Snow (1827, 1863); 0724 Cryosphere: Ice Cores (4932) Keywords: hydrogen peroxide, methylhydroperoxide, Antarctica, air-snow exchange, stratospheric ozone, atmospheric oxidation capacity

Frey, Markus M.↗
NASA NTRS1994

Aerosol particles in the upper troposphere and lower stratosphere: Elemental composition and morphology of individual particles in northern midlatitudes

Atmospheric particles were collected in the midlatitude upper troposphere (UT) and lower stratosphere (LS) by inetrial impaction for subsequent electron microscopy and individual particle element analysis. More than 97% of particles analyzed on impactor substrates exposed in the LS contained only O and S in detectable quantities; these particles are believed to be acidic sulfate. Nonsulfate materials seen in the remaining particles included soot, other c-rich substances and crustal materials. Although not predominantly sulfate, usually carried a sulfer-rich coating in the LS. Samples collected very near and just below the tropopause were also dominated by sulfates. The fraction of sulfate particles analyzed on impactor substrates exposed in the UT was 91-94% of the total particle concentration. Nonsulfate substances observed in the UT samples included crustal-type material, hydrated marine salts, carbon-rich materials of several types, and metal-containing substances of uncertain origin. Most of these UT particles were not coated with detectable quantitites of sulfate.

Sheridan, Patrick J.↗
NASA NTRS1980

Response of the global climate to changes in atmospheric chemical composition due to fossil fuel burning

Recent modeling of atmospheric chemical processes (Logan et al, 1978; Hameed et al, 1979) suggests that tropospheric ozone and methane might significantly increase in the future as the result of increasing anthropogenic emissions of CO, NO(x), and CH4 due to fossil fuel burning. Since O3 and CH4 are both greenhouse gases, increases in their concentrations could augment global warming due to larger future amounts of atmospheric CO2. To test the possible climatic impact of changes in tropospheric chemical composition, a zonal energy-balance climate model has been combined with a vertically averaged tropospheric chemical model. The latter model includes all relevant chemical reactions which affect species derived from H2O, O2, CH4, and NO(x). The climate model correspondingly incorporates changes in the infrared heating of the surface-troposphere system resulting from chemically induced changes in tropospheric ozone and methane. This coupled climate-chemical model indicates that global climate is sensitive to changes in emissions of CO, NO(x) and CH4, and that future increases in these emissions could augment global warming due to increasing atmospheric CO2.

Hameed, S.↗
NASA NTRS2019

Trends in Global Tropospheric Ozone Inferred from a Composite Record of TOMS/OMI/MLS/OMPS Satellite Measurements and the MERRA-2 GMI Simulation

Past studies have suggested that ozone in the troposphere has increased globally throughout much of the 20th century due to increases in anthropogenic emissions and transport. We show, by combining satellite measurements with a chemical transport model, that during the last four decades tropospheric ozone does indeed indicate increases that are global in nature, yet still highly regional. Satellite ozone measurements from Nimbus-7 and Earth Probe Total Ozone Mapping Spectrometer (TOMS) are merged with ozone measurements from the Aura Ozone Monitoring Instrument/Microwave Limb Sounder (OMI/MLS) to determine trends in tropospheric ozone for 1979–2016. Both TOMS (1979–2005) and OMI/MLS (2005–2016) depict large increases in tropospheric ozone from the Near East to India and East Asia and further eastward over the Pacific Ocean. The 38-year merged satellite record shows total net change over this region of about +6 to +7 Dobson units (DU) (i.e., ∼15 %–20 % of average background ozone), with the largest increase (∼4 DU) occurring during the 2005–2016 Aura period. The Global Modeling Initiative (GMI) chemical transport model with time-varying emissions is used to aid in the interpretation of tropospheric ozone trends for 1980–2016. The GMI simulation for the combined record also depicts the greatest increases of +6 to +7 DU over India and East Asia, very similar to the satellite measurements. In regions of significant increases in tropospheric column ozone (TCO) the trends are a factor of 2–2.5 larger for the Aura record when compared to the earlier TOMS record; for India and East Asia the trends in TCO for both GMI and satellite measurements are ∼+3 DU decade(exp −1) or greater during 2005–2016 compared to about +1.2 to +1.4 DU decade(exp −1) for 1979–2005. The GMI simulation and satellite data also reveal a tropospheric ozone increases in ∼+4 to +5 DU for the 38-year record over central Africa and the tropical Atlantic Ocean. Both the GMI simulation and satellite-measured tropospheric ozone during the latter Aura time period show increases of ∼+3 DU decade−1 over the N Atlantic and NE Pacific.

Ziemke, Jerald R.↗
NASA NTRS2007

Importance of Rain Evaporation and Continental Convection in the Tropical Water Cycle

Atmospheric moisture cycling is an important aspect of the Earth's climate system, yet the processes determining atmospheric humidity are poorly understood. For example, direct evaporation of rain contributes significantly to the heat and moisture budgets of clouds, but few observations of these processes are available. Similarly, the relative contributions to atmospheric moisture over land from local evaporation and humidity from oceanic sources are uncertain. Lighter isotopes of water vapour preferentially evaporate whereas heavier isotopes preferentially condense and the isotopic composition of ocean water is known. Here we use this information combined with global measurements of the isotopic composition of tropospheric water vapour from the Tropospheric Emission Spectrometer (TES) aboard the Aura spacecraft, to investigate aspects of the atmospheric hydrological cycle that are not well constrained by observations of precipitation or atmospheric vapour content. Our measurements of the isotopic composition of water vapour near tropical clouds suggest that rainfall evaporation contributes significantly to lower troposphere humidity, with typically 20% and up to 50% of rainfall evaporating near convective clouds. Over the tropical continents the isotopic signature of tropospheric water vapour differs significantly from that of precipitation, suggesting that convection of vapour from both oceanic sources and evapotranspiration are the dominant moisture sources. Our measurements allow an assessment of the intensity of the present hydrological cycle and will help identify any future changes as they occur.

Worden, John↗
NASA NTRSDate not supplied

Long-range Transport of Siberian Biomass Burning Emissions to North America During FIREX-AQ

Biomass burning from wildfires is a significant global source of aerosol and trace gases which impact air quality, tropospheric and stratospheric composition, and climate. During the summer of 2019, wildfire activity in central and eastern Siberia occurred during the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) campaign conducted between July 24 and September 6, 2019. Ground-based lidar observations from the Autonomous Mobile Ozone Lidar for Tropospheric Experiments (AMOLITE) system in Alberta, Canada retrieved frequent anomalous ozone (O3) and aerosol lamina in the troposphere and lower stratosphere during this campaign. Data from NASA’s GEOS Composition Forecast (GEOS-CF) coupled chemistry meteorology model, TROPOspheric Monitoring Instrument (TROPOMI), Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO), and ground-based insitu data were used to define the trans-Pacific and trans-Arctic transport pathway of Siberian biomass burning emissions resulting in the enhanced O3 and aerosol lamina observed by AMOLITE in western Canada. Siberian wildfires impacted North American air quality resulting in enhancements of hourly-averaged surface carbon monoxide (CO) (total CO >150 ppb) and fine particulate matter (PM2.5) (>20 μg m-3) in western Canada, however, minimal increases in surface-level O3 were measured as well as modeled by GEOS-CF. The impact in western Canada due to Siberian wildfires was much larger in the free troposphere, demonstrated by GEOS-CF and AMOLITE O3 lamina 30–40 ppb above background values and model-predicted PM2.5 lamina >30 μg m-3. In addition to tropospheric composition effects, the large wildfire activity in Siberia may have influenced the stratosphere as data from AMOLITE, CALIPSO, and GEOS-CF all suggested aerosol layers from the fires were located 13–18 km above ground level (agl). This study shows that the Siberian biomass burning emissions in the summer of 2019 impacted tropospheric/stratospheric composition in western Canada, and potentially could have influenced areas in the vicinity of FIREX-AQ airborne measurements, and future studies of FIREX-AQ chemical composition should consider how this long-range transport could have influenced the background trace gas and aerosol concentrations being investigated.

Biomass↗
NASA NTRS1999

Shipboard and Satellite Views of Elevated Tropospheric Ozone over the Tropical Atlantic in January-February 1999

During the Aerosols99 trans-Atlantic cruise from Norfolk, VA, to Cape Town, South Africa, daily ozonesondes were launched from the NOAA R/V Ronald H Brown between 17 January and 6 February l999. A composite of tropospheric ozone profiles along the latitudinal transect shows 4 zones, which are interpreted using correlative shipboard ozone, CO, water vapor, and overhead aerosol optical thickness measurements. Elevated ozone associated with biomass burning north of the ITCZ (Intertropical Convergence Zone) is prominent at 3-5 km from 10-0N, but even higher ozone (100 ppbv, 7-10 km) occurred south of the ITCZ, where it was not burning. Column-integrated tropospheric ozone was 44 Dobson Units (DU) in one sounding, 10 DU lower than the maximum in a January-February 1993 Atlantic cruise with ozonesondes [Weller et al., 1996]. TOMS tropospheric ozone shows elevated ozone extending throughout the tropical Atlantic in January 1999. Several explanations are considered. Back trajectories, satellite aerosol observations and shipboard tracers suggest a combination of convection and interhemispheric transport of ozone and/or ozone precursors, probably amplified by a lightning NO source over Africa.

Thompson, Anne M.↗
NASA NTRS2005

Chemistry, Dynamics, and Radiation of Ozone Loss: Airborne Measurements of OH, HO2, NO2, ClO, BrO, IO, ClONO2, BrONO2, ClOOCl, and H2O

This grant continued the research initially funded under NAG1-01095. This research addresses, through a combination of in situ and remote aircraft-borne instruments, the following scientific questions: Which mechanisms are responsible for the continuing erosion of ozone over midlatitudes of the Northern Hemisphere? Will the rapid loss of ozone over the Arctic in late winter continue to worsen over the next two decades? Are these large losses dynamically coupled to midlatitudes? Which mechanisms dictate the rate of exchange of material between the troposphere and stratosphere? How will these processes change in response to changes in climate? Will regional scale pollution episodes, that are emerging as predictable seasonal events, significantly affect the middle-to-upper troposphere chemical composition. If so, how will these changes alter the chemical composition of the middle world? What changes are predicted for the overworld? Why has the arctic stratosphere become colder in the late winter phase in recent years? Have increases in tropical upper troposphere temperatures increased the temperature gradient such as to change the trajectories of vertically propagating waves, thus reducing the effectiveness of the meridional circulation for transport of heat, momentum and ozone from the tropics to high latitudes?

Anderson, James G.↗
NASA NTRS2005

Chemistry, Dynamics, and Radiation of Ozone Loss: Airborne Measurements of OH, HO2, N02, Cl0, BrO, IO, ClON02, BrON02, CIOOCl, and H2O

This research addresses, through a combination of in situ and remote aircraft-borne Which mechanisms are responsible for the continuing erosion of ozone over midlatitudes of the Northern Hemisphere? Will the rapid loss of ozone over the Arctic in late winter continue to worsen over the next two decades? Are these large losses dynamically coupled to midlatitudes? Which mechanisms dictate the rate of exchange of material between the troposphere and stratosphere? How will these processes change in response to changes in climate? Will regional scale pollution episodes, that are emerging as predictable seasonal events, significantly affect the middle-to-upper troposphere chemical composition. If so, how will these changes alter the chemical composition of the middle world? What changes are predicted for the overworld? Why has the arctic stratosphere become colder in the late winter phase in recent years? Have increases in tropical upper troposphere temperatures increased the temperature gradient such as to change the trajectories of vertically propagating waves, thus reducing the effectiveness of the meridional circulation for transport of heat, momentum and ozone from the tropics to high latitudes?

Anderson, James G.↗
NASA NTRS1982

Importance of heterogeneous processes to tropospheric chemistry - Studies with a one-dimensional model

A one-dimensional, time-dependent model of tropospheric air composition is developed which incorporates several heterogeneous physical and chemical processes. The model includes the interaction of gases, aerosols, and hydrometeors through the physical mechanisms of nucleation, condensation, evaporation, coagulation, coalescence, and deliquescence. Precipitation, sedimentation, and dry deposition act to remove material from the atmosphere, while chemical transformations occur both in the vapor and the condensed phases. The model also incorporates the sources and vertical diffusion of gases and particles, as well as changes in the solar intensity caused by light-scattering from aerosols and clouds. Preliminary simulations made using this model indicate that rainout and washout processes strongly influence the distributions of tropospheric gases and aerosols under certain conditions.

Turco, R. P.↗
NASA NTRS2003

Intercomparisons of Airborne Measurements of Aerosol Ionic Chemical Composition during TRACE-P and ACE-Asia

As part of the two field studies, Transport and Chemical Evolution over the Pacific (TRACE-P), and the Asian Aerosol Characterization Experiment (ACEAsia), the inorganic chemical composition of tropospheric aerosols was measured over the western Pacific from three separate aircraft using various methods. Comparisons are made between the rapid online techniques of the Particle Into Liquid Sampler (PILS) for measurement of a suite of fine particle ionic compounds and a mist chamber (MC/IC) measurement of fine sulfate, and the longer time-integrated filter and multi-orifice impactor (MOI) measurements. Comparisons between identical PILS on two separate aircraft flying in formation showed that they were highly correlated (e.g., sulfate r(sup 2) of 0.95), but were systematically different by 10 +/- 5% (linear regression slope and 95% confidence bounds), and had generally higher concentrations on the aircraft with a low turbulence inlet and shorter inlet-to-instrument transmission tubing. Comparisons of PILS and mist chamber measurements of fine sulfate on two different aircraft during formation flying had an 3 of 0.78 and a relative difference of 39% +/- 5%. MOI ionic data integrated to the PILS upper measurement size of 1.3 pm sampling from separate inlets on the same aircraft showed that for sulfate, PILS and MOI were within 14% +/- 6% and correlated with an r(sup 2) of 0.87. Most ionic compounds were within f 30%, which is in the range of differences reported between PILS and integrated samplers from ground-based comparisons. In many cases, direct intercomparison between the various instruments is difficult due to differences in upper-size detection limits. However, for this study, the results suggest that the fine particle mass composition measured from aircraft agree to within 30-40%.

Ma, Y.↗
NASA NTRS1973

Chemistry of the lower atmosphere

The presence of particulate matter in the lower atmosphere is considered, giving attention to the sources of particles in the troposphere, the composition of particles collected from the atmosphere, aspects of particle concentrations and size distributions, mechanisms of removal, residence times, and conditions in the lower stratosphere. The role of natural and anthropogenic pollutants in cloud and precipitation formation is discussed together with removal processes of gaseous and particulate pollutants, and the global sulfur cycle. Other topics examined include the chemical basis for climatic change and the carbon dioxide cycle. Individual items are announced in this issue.

Rasool, S. I.↗
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.↗