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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 NTRS1980

Evaluated kinetic and photochemical data for atmospheric chemistry

This paper contains a critical evaluation of the kinetics and photochemistry of gas phase chemical reactions of neutral species involved in middle atmosphere chemistry (10-55 km altitude). Data sheets have been prepared for 148 thermal and photochemical reactions, containing summaries of the available experimental data with notes giving details of the experimental procedures. For each reaction a preferred value of the rate coefficient at 298 K is given together with a temperature dependency where possible. The selection of the preferred value is discussed, and estimates of the accuracies of the rate coefficients and temperature coefficients have been made for each reaction. The data sheets are intended to provide the basic physical chemical data needed as input for calculations which model atmospheric chemistry. A table summarizing the preferred rate data is provided, together with an appendix listing the available data on enthalpies of formation of the reactant and product species.

Baulch, D. L.↗
NASA NTRS1981

Photochemical processes induced by a major warming of the upper atmosphere - Variations in mesospheric trace constituents

The temperature rise and enhanced winds during an upper atmospheric warming cause substantial changes in the high level ozone profile of the sunlit winter hemisphere. Calculations based on a photochemical model, using temperatures measured at Fort Churchill during a major warming, predict a factor of 2 variation in the ozone number density near 60 km over a time period of approximately 3 weeks. This temporal variability at a fixed location results from the planetary wave structure of the temperature field and reflects a similar longitudinal behavior at a given time. The ozone number density at fixed altitude is a maximum when the temperature is greatest at and below this level. This is due primarily to thermal expansion of the atmosphere which results in a large increase in pressure at constant altitude. However, chemical activity during a warming decreases the mesospheric ozone mixing ratio at fixed pressure. The ozone mixing ratio at constant pressure during the peak of the event studied is near 75% of its unperturbed value. The predicted variability of ozone in longitude and time demonstrates the need for hemispheric scale information on trace gas abundances, temperature, and winds in order to delineate adequately the response of upper atmospheric composition to a major perturbation.

Frederick, J. E.↗
NASA NTRS1981

The transport of photochemical pollutants to the background troposphere

The considered investigation is concerned with the phenomena occurring as a chemically reacting plume, with specific initial concentrations of NO, NO2, O3, and hydrocarbons, emerges from an urban area and is advected to the background troposphere. A better understanding of the global NOx and hydrocarbon budgets can be realized by determining the fractions of NOx and hydrocarbons that are transported to distances far enough to be considered background. The investigation makes use of a 56-step, lumped kinetic mechanism for photochemical smog, which includes current information on pertinent chemical reactions and rate constants for the reactions.

Bazzell, C. C.↗
NASA NTRS1981

Laboratory measurements of the cometary photochemical phenomena

Laboratory experiments are described that provide fundamental information about photochemical processes in comets. The yield of cometary radicals such as CN, OH, etc. can be determined as a function of photolyzing wavelength. Quantum state distributions of the internal energy of the cometary radicals can also be measured as a function of wavelength permitting one to define the recoil velocity of the fragments. This type of information supplies the data needed for more elaborate models to interpret the data being obtained on comets.

Jackson, W. M.↗
NASA NTRS1981

Production of hydrogen by electron transfer catalysis using conventional and photochemical means

Alternate methods of generating hydrogen from the sulfuric acid thermal or electrochemical cycles are presented. A number of processes requiring chemical, electrochemical or photochemical methods are also presented. These include the design of potential photoelectrodes and photocatalytic membranes using Ru impregnated nafion tubing, and the design of experiments to study the catalyzed electrolytic formation of hydrogen and sulfuric acid from sulfur dioxide and water using quinones as catalysts. Experiments are carried out to determine the value of these approaches to energy conversion.

Rillema, D. P.↗
NASA NTRS1981

The feasibility of using time-dependent photochemical calculations to infer radical species concentrations from solar occultation absorption measurements

In connection with fast chemical reactions, short-lived stratospheric species experience rapid concentration variations at sunset and sunrise. For solar occultation absorption measurements, these rapid concentration variations may introduce significant errors with respect to the inference of atmospheric abundances for some species due to asymmetrical concentration distributions. Most retrieval algorithms assume that concentration distributions are spherically symmetric. The effect of this assumption on the accuracy of inferred concentrations has been studied by Kerr et al. (1977). The present investigation considers the feasibility of using a time-dependent one-dimensional photochemical model to provide detailed information about the asymmetrical distribution for use in the retrieval procedure. As shown by Boughner et al. (1980), diurnal effects can be represented by an inhomogeneity factor. It is found that the NO retrieval improves considerably with the inclusion of a correction factor containing the asymmetrical variations.

Larsen, J. C.↗
NASA NTRS1982

Laboratory studies of photochemical and spectroscopic phenomena related to comets

The relationship between laboratory observations and cometary phenomena is reviewed, with particular attention to how laboratory studies must be done to obtain all data needed for astronomical purposes. It is pointed out how supersonic expansion of the gas evaporating from the nucleus can affect the photochemical lifetime and the energy partitioning among the fragments. The use of the CS radical as a remote sensing probe of conditions in the inner coma is also discussed.

Jackson, W. M.↗
NASA NTRS1983

The application of forest classification from Landsat data as a basis for natural hydrocarbon emission estimation and photochemical oxidant model simulations in southeastern Virginia

The possible contribution by natural hydrocarbon emissions to the total ozone budget recorded in the Tidewater region of southeastern Virginia during the height of the summer period was examined. Natural sources investigated were limited to the primary HC emitters and most prevalent natural vegetation, the forests. Three types and their areal coverage were determined for Region VI of the Virginia State Air Pollution Control Board using remotely sensed data from Landsat, a NASA experimental earth resources satellite. Emission factors appropriate to the specific types (coniferous 0.24 x 10 to the 13th, mixed 0.63 x 10 to the 13th, deciduous 1.92 x 10 to the 13th, microgram/h), derived from contemporary procedures, were applied to produce an overall regional emission rate of 2.79 x 10 to the 13th microgram/h for natural non-methane hydrocarbons (NMHC). This rate was used with estimates of the anthropogenic NO(x) and NMHC loading, as input into a photochemical box model. Additional HC loading on the order of that estimated to be produced by the natural forest communities was required in order to reach certain measured summer peak ozone levels as the computer simulation was unable to account for the measured episodic levels on the basis of the anthropogenic inventory alone.

Salop, J.↗
NASA NTRS1983

Photochemical synthesis of biomolecules under anoxic conditions

The long-wavelength UV anoxic photosynthesis of uracil, various sugars (including deoxyribose and glycoaldehyde), amino acids, and other organic photoproducts is reported. The reactions were conducted in a mixture of water, calcium carbonate, hydrazine, and formaldehyde which were subjected to 24 hr or 72 hr radiation. Product yields were greatest when the hydrazine/formaldehyde ratio was one, and when the reactant concentrations were low. These data suggest that organic products can be formed in variety from those amounts of formaldehyde and hydazine precursors which are themselves formed under anoxic UV photochemical conditions.

Folsome, C.↗
NASA NTRS1983

A two-dimensional photochemical model of the atmosphere. I Chlorocarbon emissions and their effect on stratospheric ozone

A two-dimensional photochemical model is used to examine changes to the ozone layer caused by emissions of CFCl3, CF2Cl2, CH3CCl3 and CCl4. The influence of a possible secular increase in tropospheric methane up to 2 percent per year was found to be small, although it acts to mask decreases in total ozone caused by the chlorocarbons. Increasing NO(x) emissions caused by industralization also tend to mask decreases in total ozone and may have caused total ozone to increase by about 1 percent. The model-calculated ozone decreases are estimated to be about 3 percent by 1980. This estimate is higher than estimates by similar models, although it is noted that CCl4 and CH3CCl3 emissions are included in the model in addition to CFCl3 and CF2Cl2. This is significant because the model indicates that CCl4 has dominated the ozone depletions so far, and knowledge of the historical emission rate of CCl4 to the atmosphere is incomplete. There remain sufficient significant disagreements between theoretical and observed concentrations and variabilities, particularly for odd nitrogen and ClO, to caution against assigning too much confidence in the calculated ozone depletion.

Gidel, L. T.↗
NASA NTRS1983

Photochemical reactions of water and carbon monoxide in earth's primitive atmosphere

The gas-phase photolysis of H2O at 1849 A in the presence of CO yields mainly CO2 and H2 and a variety of organic compounds, including C1-C3 hydrocarbons, alcohols, aldehydes, acetone, and acetic acid. The overall quantum yield for conversion of CO to organic compounds varies between 0.23 and 0.03 as a function of the CO abundance. These results indicate that even if primitive earth's atmosphere initially contained no molecular hydrogen and contained carbon only in the form of CO or a mixture of CO and CO2, the prebiotic environment would have become enriched with a variety of organic compounds produced by photochemical processes.

Bar-Nun, A.↗
NASA NTRS1984

Stratospheric NO and NO2 profiles at sunset from analysis of high-resolution balloon-borne infrared solar absorption spectra obtained at 33 deg N and calculations with a time-dependent photochemical model

Simultaneous stratospheric vertical profiles of NO and NO2 at sunset were derived from an analysis of infrared solar absorption spectra recorded from a float altitude of 33 km with an interferometer system during a balloon flight. A nonlinear least squares procedure was used to analyze the spectral data in regions of absorption by NO and NO2 lines. Normalized factors, determined from calculations of time dependent altitude profiles with a detailed photochemical model, were included in the onion peeling analysis to correct for the rapid diurnal changes in NO and NO2 concentrations with time near sunset. The CO2 profile was also derived from the analysis and is reported.

Rinsland, C. P.↗
NASA NTRS1982

Natural hydrocarbon emission estimates based on Landsat data as an input to a regional ozone photochemical model

Landsat-derived forest cover data were employed with non-methane hydrocarbon (NMHC) emission rates in a model to quantify summer forest ozone production for the Tidewater Region of Virginia. The areal extent of the three major forest types - coniferous, deciduous, and mixed - were determined from Landsat data on two adjacent scenes, using an unsupervised approach to spectral signature development. The forest type results from both data sets were verified in an extensive accuracy assessment and merged to provide regional statistics for total acreages, percent forest, and error rates. The Landsat statistics were incorporated into forest type emission factor equations to produce an estimated emission rate for natural hydrocarbons from forests. This estimate, along with measured rates for nitrogen oxides and NMHC from anthropogenic sources, was provided as input to computer simulations of atmospheric ozone generation for the Tidewater Region using a photochemical oxident model.

Middleton, E. M.↗
NASA NTRS1984

A diabatic circulation experiment in a two-dimensional photochemical model

A two-dimensional photochemical model based on diabatic circulation has been used to simulate the behavior of N2O, CFCl3(F-11) and CF2Cl2(F-12) The circulation is based on estimates of net heating from the ground to 60 km. Eddy diffusion has been reduced with respect to other model studies with Kzz = 2000 sq cm/s everywhere bove 100 mbar. Resulting tracer profiles show reasonable agreement with measured profiles in the tropics and fall off much more sharply with altitude than those produced by models using larger values of Kzz. The agreement obtained is at least as good as that obtained with adjustable, eddy diffusion parameters. The diabatic circulation treatment is more closely related to related to real physical processes and thus more easily interpreted. Diffusive mixing appears to be more important in determining the details of the tracer distributions than the basic morphology.

Guthrie, P. D.↗
NASA NTRS1984

Diurnal variations of atmospheric nitric oxide - Ground-based infrared spectroscopic measurements and their interpretation with time-dependent photochemical model calculations

Total vertical column amounts of NO have been derived from infrared solar absorption spectra recorded near sunrise and sunset with the 0.01 per cm resolution Fourier transform interferometer at the national Solar Observatory on Kitt peak (elevation 2095 m, latitude 31.9 degrees N) on February 23, 1981. The results show an increase in NO concentration in the morning, late afternoon values about 40 percent higher than in the morning, and a decrease in NO concentration prior to sunset. The measured diurnal changes in the total vertical column amount are compared with values obtained from time-dependent photochemical calculations.

Rinsland, C. P.↗