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At least 145 records · Page 8

Exploring Oxidation in the Remote Free Troposphere: Insights From Atmospheric Tomography (ATom)

Earth's atmosphere oxidizes the greenhouse gas methane and other gases, thus determining their lifetimes and oxidation products. Much of this oxidation occurs in the remote, relatively clean free troposphere above the planetary boundary layer, where the oxidation chemistry is thought to be much simpler and better understood than it is in urban regions or forests. The NASA airborne Atmospheric Tomography study (ATom) was designed to produce cross sections of the detailed atmospheric composition in the remote atmosphere over the Pacific and Atlantic Oceans during four seasons. As part of the extensive ATom data set, measurements of the atmosphere's primary oxidant, hydroxyl (OH), and hydroperoxyl (HO2) are compared to a photochemical box model to test the oxidation chemistry. Generally, observed and modeled median OH and HO2 agree to within combined uncertainties at the 2σ confidence level, which is ~±40%. For some seasons, this agreement is within ~±20% below 6-km altitude. While this test finds no significant differences, OH observations increasingly exceeded modeled values at altitudes above 8 km, becoming ~35% greater, which is near the combined uncertainties. Measurement uncertainty and possible unknown measurement errors complicate tests for unknown chemistry or incorrect reaction rate coefficients that would substantially affect the OH and HO2 abundances. Future analysis of detailed comparisons may yield additional discrepancies that are masked in the median values.

atmosphere's primary oxidant, hydroxyl (OH), and h↗

Surface-catalyzed air oxidation reactions of hydrazines: Tubular reactor studies

The surface-catalyzed air oxidation reactions of hydrazine, monomethylhydrazine, unsymmetrical dimethylhydrazine, symmetrical dimethylhydrazine, trimethylhydrazine and tetramethylhydrazine were investigated in a metal-powder packed turbular flow reactor at 55 plus or minus 3 C. Hydrazine was completely reacted on all surfaces studied. The major products of monomethylhydrazine (MMH) oxidation were methanol, methane and methyldiazene. The di-, tri- and tetra-methyl hydrazines were essentially unreactive under these conditions. The relative catalytic reactivities toward MMH are: Fe greater than Al2O3 greater than Ti greater than Zn greater than 316 SS greater than Cr greater than Ni greater than Al greater than 304L SS. A kinetic scheme and mechanism involving adsorption, oxidative dehydrogenation and reductive elimination reactions on a metal oxide surface are proposed.

Kilduff, Jan E.↗

Register of specialized sources for information on selected fuels and oxidizers

Thirty-eight (38) organizations are listed and described that catalog and file information in their data systems on fuel and oxidizers. The fuels include hydrogen, methane and hydrazine-type fuels; the oxidizers include oxygen, fluorine, flox, nitrogen tetroxide and ozone. The type of available information covers thermophysical properties, propellant systems, propellant fires-control-extinguishment, propellant explosions, propellant combustion, propellant safety, and fluorine chemistry. These organizations have assembled and collated their information so that it will be useful in the solution of engineering problems.

Ludtke, P. R.↗

Global and Regional Temperature-change Potentials for Near-term Climate Forcers

The emissions of reactive gases and aerosols can affect climate through the burdens of ozone, methane and aerosols, having both cooling and warming effects. These species are generally referred to near-term climate forcers (NTCFs) or short-lived climate pollutants (SLCPs), because of their short atmospheric residence time. The mitigation of these would be attractive for both air quality and climate on a 30-year timescale, provided it is not at the expense of CO2 mitigation. In this study we examine the climate effects of the emissions of NTCFs from 4 continental regions (East Asia, Europe, North America and South Asia) using results from the Task Force on Hemispheric Transport of Air Pollution Source-Receptor global chemical transport model simulations. We address 3 aerosol species (sulphate, particulate organic matter and black carbon - BC) and 4 ozone precursors (methane, reactive nitrogen oxides - NOx, volatile organic compounds VOC, and carbon monoxide - CO). For the aerosols the global warming potentials (GWPs) and global temperature change potentials (GTPs) are simply time-dependent scaling of the equilibrium radiative forcing, with the GTPs decreasing more rapidly with time than the GWPs. While the aerosol climate metrics have only a modest dependence on emission region, emissions of NOx and VOCs from South Asia have GWPs and GTPs of higher magnitude than from the other northern hemisphere regions. On regional basis, the northern mid-latitude temperature response to northern mid-latitude emissions is approximately twice as large as the global average response for aerosol emission, and about 20-30% larger than the global average for methane, VOC and CO emissions. We also found that temperatures in the Arctic latitudes appear to be particularly sensitive to black carbon emissions from South Asia.

climate forcer↗

Molecular absorption parameters in atmospheric modelling

Molecular spectroscopic parameters are compiled for a number of infrared-active molecules occurring naturally in the terrestrial atmosphere. The following molecules are included in this compilation: water vapor; carbon dioxide; ozone; nitrous oxide; carbon monoxide; methane; and oxygen. The spectral region covered extends from less than 1 micron to the far infrared, and data are presented on more than 100,000 spectral lines. The parameters included in the compilation for each line are: frequency, intensity, half-width, energy of the lower state of the transition, vibrational and rotational identifications of the upper and lower energy states, an isotopic identification, and a molecular identification. Using this data compilation, band model parameters are presented for water vapor, carbon dioxide, and ozone averaged over 20 wavenumber intervals. Using these parameters in a random model formulation, transmittance spectra are provided and compared with both degraded monochromatic calculations and laboratory data.

Mcclatchey, R. A.↗

The NASA Ames Research Center one- and two-dimensional stratospheric models. Part 1: The one-dimensional model

A one-dimensional model of stratospheric trace constituents is described in detail. Specifically, the numerical solution of the species continuity equations, including a technique for treating the stiff differential equations representing the chemical kinetic terms, and an appropriate method for simulating the diurnal variations of the species concentrations, are discussed. A specialized treatment of atmospheric photodissociation rates is outlined in the text. The choice of a vertical eddy diffusivity profile and its success in predicting the vertical tracer distributions (carbon 14, methane, and nitrous oxide) are also discussed.

Turco, R. P.↗

Non Urban Troposphere Composition Symposium, Hollywood, Fla., November 10-12, 1976, Proceedings

Papers are presented which originate from a conference on 'The Non-Urban Troposphere Composition', held in 1976. Attention is given to distributions of nitrous oxide in the atmosphere, and to tropospheric and stratospheric compositions which are perturbed by NO(x) emissions from high-altitude aircraft. Ozone is studied in terms of in situ measurements; various meteorological analyses of tropopause folding, ozone measurements in the Boston area, and ozone measurements in rural areas are presented. A one-dimensional model used to study tropospheric photochemistry numerically is presented as are vertical profiles of tropospheric and stratospheric molecular hydrogen. The oxidation of ammonia, methane, and hydrogen sulfide is assessed in nonurban tropospheres along with nonurban measurements of ethane and methane for various atmospheric conditions. With reference to the particle size distribution of chloride in the marine aerosol, organic and inorganic chlorine concentrations are evaluated, and measurements of sea-air CO2 flux by eddy correlation are investigated.

Source record↗

Summary of southeastern Virginia urban plume measurement data for August 4 and 5, 1977

The measurement program was conducted to define the characteristics of the Southeastern Virginia urban plume with emphasis on the photooxidant species. The measurement area was a rectangle approximately 200 km by 60 km centered in the Hampton Roads area of Tidewater Virginia. This area includes the cities of Norfolk, Virginia Beach, Chesapeake, Newport News, and Hampton. The data set presented includes aircraft measurements for ozone, nitrogen oxides, carbon monoxide, methane, and meteorological parameters such as dewpoint temperature. Surface level data for ozone are presented for 10 stations located throughout the test area. Comprehensive meteorological data from existing National Weather Service stations and special locations selected for the urban plume program are summarized.

Gregory, G. L.↗

Meridional distribution of stratospheric trace constituents

Vertically stratified tracers such as methane and nitrous oxide tend to have constant mixing ratio surfaces that slope downward toward the poles in the meridional plane. The equilibrium tracer slope results from the competition between the slope steepening effects of advection by the diabatic circulation and the slope flattening effects of quasi-isentropic eddy transport and photochemical loss. The diabatic circulation iself is, however, driven primarily by eddy transports, which maintain the departure of stratospheric temperatures from radiative equilibrium. If the eddy transports are weak, the diabatic circulation is also weak and the slope is small. Using a simple beta-plane channel model and an eddy diffusion parameterization for the eddy potential vorticity and tracer transports, it is shown that the slope is a maximum for a value of eddy diffusion such that the dynamical time scale lies between the radiative and chemical time scales.

Holton, J. R.↗

The potential impact on atmospheric ozone and temperature of increasing trace gas concentrations

The response of the atmosphere to emissions of chlorofluorocarbons (CFCs) and other chlorocarbons, and to increasing concentrations of other radiatively active trace gases such as CO2, CH4, and N2O is calculated by a coupled chemical-radiative transport one-dimensional model. It is shown that significant reductions in the ozone concentration and in the temperature are expected in the upper stratosphere as a result of increasing concentrations of active chlorine produced by photodecomposition of the CFCs. The ozone content is expected to increase in the troposphere, as a consequence of increasing concentrations of methane and nitrogen oxides. Due to enhanced greenhouse effects, the Earth's surface should warm up by several degrees. The amplitude and even the sign of future changes in the ozone column are difficult to predict as they are strongly scenario-dependent. An early detection system to prevent noticeable ozone changes as a result of increasing concentrations of source gases should thus be based on a continuous monitoring of the ozone amount in the upper stratosphere rather than on measurements of the ozone column only. Measurements of NOx, Clx, and HOx are also required for unambiguous trend detection and interpretation.

Brasseur, G.↗

Nimbus-7 Stratospheric and Mesospheric Sounder (SAMS) experiment data user's guide

The Stratospheric and Mesospheric Sounder (SAMS) aboard Nimbus-7 observes infrared radiation from the atmospheric limb. Global upper atmosphere temperature profiles and vertical concentrations of H2O, NO, N2O, CH4 and CO2 are derived from these measurements. The status of all channels was carefully monitored. Temperature and composition were retrieved from the measurements by linearizing the direct equation about an a priori profile and using an optimum statistical estimator to find the most likely solution. The derived temperature and composition profiles are archived on two tape products whose file structure and record formats are described in detail. The gridded retrieved temperature tape (GRID-T) contains daily day and night average temperatures at 62 pressure levels in a 2.5 degree latitude by 10 degree longitude grid extending from 67.5 degrees N to 50 degrees S. The zonal mean methane and nitrous oxide composition tape (ZMT-G) contains zonal mean day and night average CH4 and N2O mixing ratios at 31 pressure levels for 2.5 degrees latitude zones extending from 67.5 degrees N to 50 degrees S.

Taylor, F. W.↗

Improved Limb Atmospheric Spectrometer (ILAS) for polar stratospheric trace gas measurements

The Improved Limb Atmospheric Spectrometer (ILAS) is a grating spectrometer designed to measure vertical profiles of high latitude stratospheric constituents in a solar occultation mode. ILAS measurement gases are ozone (03), methane (CH4), nitrous oxide (N2O), nitric acid (HNO3), water vapor (H2O), nitrogen dioxide (NO2), and CFC-11 using an IR channel. Temperature, pressure, and aerosol are also measured using a visible channel. The IR channel consists of 44 detector elements which cover the spectral range 6.2 to 11.8 microns, and the visible channel is composed of 1024 pixels that cover 753 to 784 nm. ILAS will be installed on the Advanced Earth Observing Satellite (ADEOS) which will be launched in 1995. Instrument design data are outlined.

Yokota, Tatsuya↗

A new numerical model of the middle atmosphere. I - Dynamics and transport of tropospheric source gases

Attention is given to a new model of the middle atmosphere which includes, in addition to the equations governing the zonal mean state, a potential vorticity equation for a single planetary-scale Rossby wave, and an IR radiative transfer code for the stratosphere and lower mesosphere, which replaces the Newtonian cooling parameterization used previously. It is shown that explicit computation of the planetary-scale wave field yields a more realistic representation of the zonal mean dynamics and the distribution of trace chemical species. Wave breaking produces a well-mixed 'surf zone' equatorward of the polar night vortex and drives a meridional circulation with downwelling on the poleward side of the vortex. This combination of mixing and downwelling produces shallow meridional gradients of trace gases in the subtropics and middle latitudes, and very steep gradients at the edge of the polar vortex. Computed distributions of methane and nitrous oxide are shown to agree well with observations.

Garcia, Rolando R.↗

Analysis of satellite-derived ozone and water vapor measurements

Research under this grant has involved analyses of satellite-derived measurements of water vapor and total ozone. Upper tropospheric water vapor data from the Nimbus 7 temperature-humidity infrared radiometer (THIR) 6.7 micron channel were analyzed by Fourier transformation to provide wavenumber spectra for a case of an upper level system over Europe. The power law spectrum for horizontal scales from 60 to several hundred km suggests that when convective cloud energy sources are not present, the enstrophy-cascading process (with variance proportional to the minus three power of wavenumber) may hold to much smaller scales than previously thought. Several investigations of the middle atmosphere (stratosphere and mesosphere) were also conducted. Slow atmospheric oscillations with periods of 1-2 months were investigated in total ozone measurements and in ionospheric data. Using one-point correlation maps and total ozone mapping spectrometer (TOMS) data, strong statistical evidence was found for the planetary-scale oscillations at these periods. A dipole-like pattern in the tropical equatorial Indian ocean-western Pacific region was documented, along with wavetrain-like patterns emanating into the extratropics. While attempting to follow the oscillations upward above stratosphere, oscillations were studied in ionospheric data (D-region radio wave absorption, in the upper mesosphere, around 80-90 km altitude). Cross-spectral analyses with solar flux data revealed that much of the observed 1-2 month variance in the ionospheric D-region was well correlated to solar variations. Further research has involved investigations of the photochemical lifetime of greenhouse gases methane and nitrous oxide. Using Nimbus 7 satellite data, a new analysis technique was employed to determine the lifetime of these gases in situ in the upper stratosphere. The lifetimes are found to be in good agreement with theoretical estimates.

Stanford, John L.↗

Remote sounding of tropospheric minor constituents

The etalon interferometer, or Fabry-Perot interferometer (FPI), with its high throughput and high spectral resolution was widely used in the remote-sensing measurements of the earth's atmospheric composition, winds, and temperatures. The most recent satellite instruments include the Fabry-Perot interferometer flown on the Dynamics Explorer-2 (DE-2) and the High Resolution Doppler Imager (HRDI) to be flown on the Upper Atmosphere Research Satellite (UARS). These instruments measure the Doppler line profiles of the emission and absorption of certain atmospheric species (such as atomic oxygen) in the visible spectral region. The successful space flight of DE-FPI and the test and delivery of UARS-HRDI demonstrated the extremely high spectral resolution and ruggedness of the etalon system for the remote sensing of earth and planetary atmospheres. Recently, an innovative FPI focal plane detection technique called the Circle-to-Line Interferometer Optical (CLIO) system was invented at the Space Physics Research Laboratory (SPRL). The CLIO simplifies the FPI focal plane detection process by converting the circular rings or fringes into a linear pattern similar to that produced by a conventional spectrometer, while retaining the throughput advantage of the etalon interferometer. CLIO makes the use of linear array detectors more practical and efficient with FPI, the combination of FPI and CLIO represents a very promising new technique for the remote sensing of the lower atmospheres of Earth, Mars, Venus, Neptune, and other planets. The Multiorder Etalon Spectrometer (MOES), as a combination of the rugged etalon and the CLIO, compares very favorably to other spaceborne optical instruments in terms of performance versus complexity. The feasibility of an advanced etalon spectrometer for the remote sensing of tropospheric trace species, particularly carbon monoxide (CO), nitrous oxide (N2O), and methane (CH4) was discussed. The etalon atmospheric spectroscopy techniques are described, instrument design and related technical issues are discussed. The primary objective is to establish the concept of atmospheric spectroscopy with the CLIO and etalon system and its applications for the measurements of tropospheric trace species analyze system requirements and performance, determine the feasibility of components and subsystem implementation with available technology, and develop inversion algorithm for retrieval simulation and data analysis.

Drayson, S. Roland↗

A two-dimensional model with coupled dynamics, radiative transfer, and photochemistry. 2: Assessment of the response of stratospheric ozone to increased levels of CO2, N2O, CH4, and CFC

The impact of increased levels of carbon dioxide (CO2), chlorofluorocarbons (CFCs), and other trace gases on stratospheric ozone is investigated with an interactive, two-dimensional model of gas phase chemistry, dynamics, and radiation. The scenarios considered are (1) a doubling of the CO2 concentration, (2) increases of CFCs, (3) CFC increases combined with increases of nitrous oxide (N2O) and methane CH4, and (4) the simultaneous increase of CO2, CFCs, N2O, and CH4. The radiative feedback and the effect of temperature and circulation changes are studied for each scenario. For the double CO2 calculations the tropospheric warming was specified. The CO2 doubling leads to a 3.1% increase in the global ozone content. Doubling of the CO2 concentrations would lead to a maximum cooling of about 12 C at 45 km if the ozone concentration were held fixed. The cooling of the stratosphere leads to an ozone increase with an associated increase in solar heating, reducing the maximum temperature drop by about 3 C. The CFC increase from continuous emissions at 1985 rate causes a 4.5% loss of ozone. For the combined perturbations a net loss of 1.3% is calculated. The structure of the perturbations shows a north-south asymmetry. Ozone losses (when expressed in terms of percent changes) are generally larger in the high latitudes of the southern hemisphere as a result of the eddy mixing being smaller than in the northern hemisphere. Increase of chlorine leads to ozone losses above 30 km altitude where the radiative feedback results in a cooler temperature and an ozone recovery of about one quarter of the losses predicted with a noninteractive model. In all the cases, changes in circulation are small. In the chlorine case, circulation changes reduce the calculated column depletion by about one tenth compared to offline calculations.

Schneider, Hans R.↗

Biogenic and anthropogenic trace gases in the atmosphere

This paper illustrates the importance of biogenic and anthropogenic trace gases for the global environment and for the climate system. The paper briefly reviews the currently available estimates of sources and strengths of the biogenic and anthropogenic gases on the global scale. One of the major concerns for the global environment is the rapid increase in the concentration of long-lived trace gases such as CO2, CH4, N2O and the chlorofluorocarbons. The trend in the carbon dioxide concentration, as a result of fossil-fuel burning, is of the order of 0.4 percent per year, and this trend is related to the CO2 uptake by the ocean and by terrestrial ecosystems, which are likely to be modified if the planet warms up in the forthcoming decades. The concentrations of methane and nitrous oxide are increasing by 0.9 and 0.25 percent per year, respectively. In the case of the most widely used chlorofluorocarbons, trends as large as 10 percent per year or more are being measured.

Brasseur, G. P.↗