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At least 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
NASA NTRS1982

Kinetics of the reaction of hydroxyl radicals with nitric acid

An extensive study was made of the reaction of hydroxyl radicals with nitric acid in a laser photolysis-resonance fluorescence system. A 266 nm laser was used to photolyze HNO3 in the temperature range 225-415 K at pressures of 20-300 torr. A temperature dependence was detected below room temperature, with a leveling off at 298 K and a wide spread in the rate constants. A pressure dependence was observed over the entire range and was more pronounced at lower temperatures. The results are noted to be in agreement with those of previous investigations. However, the wide range of rate constants are suggested to be a problem for stratospheric HO(x) modeling for anthropogenic effects. No explanation could be given of the varying results obtained by other investigators regarding the kinetics of the reactions.

Margitan, J. J.↗
NASA NTRS1983

New technological developments for the remote detection of atmospheric hydroxyl radicals

New developments in the areas of narrowband tunable excimer lasers, high-resolution high-rejection optical filters, and wavelength measurement devices are considered for application to the remote sensing of atmospheric hydroxyl radicals. The conclusion is that an increase in the SNR of 10,000 could readily be gained through the use of these new devices. Also, considerable reductions in size and electrical energy consumption could be realized.

Mcdermid, I. S.↗
NASA NTRS1984

An intercomparison of carbon monoxide, nitric oxide, and hydroxyl measurement techniques - Overview of results

Results from an intercomparison of methods to measure carbon monoxide (CO), nitric oxide (NO), and the hydroxyl radical (OH) are discussed. The intercomparison was conducted at Wallops Island, Virginia, in July 1983 and included a laser differential absorption and three grab sample/gas chromatograph methods for CO, a laser-induced fluorescence (LIF) and two chemiluminescence methods for NO, and two LIF methods and a radiocarbon tracer method for OH. The intercomparison was conducted as a field measurement program involving ambient measurements of CO (150-300 ppbv) and NO (10-180 pptv) from a common manifold with controlled injection of CO in incremental steps from 20 to 500 ppbv and NO in steps from 10 to 220 pptv. Only ambient measurements of OH were made. The agreement between the techniques was on the order of 14 percent for CO and 17 percent for NO. Hardware difficulties during the OH tests resulted in a data base with insufficient data and uncertanties too large to permit a meaningful intercomposition.

Hoell, J. M.↗
NASA NTRS1985

An ab initio investigation of possible intermediates in the reaction of the hydroxyl and hydroperoxyl radicals

Ab initio quantum chemical techniques are used to investigate covalently-bonded and hydrogen-bonded species that may be important intermediates in the reaction of hydroxyl and hydroperoxyl radicals. Stable structures of both types are identified. Basis sets of polarized double zeta quality and large scale configuration interaction wave functions are utilized. Based on electronic energies, the covalently bonded HOOOH species is 26.4 kcal/mol more stable than the OH and HO2 radicals. Similarly, the hydrogen bonded HO---HO2 species has an electronic energy 4.7 kcal/mol below that of the component radicals, after correction is made for the basis set superposition error. The hydrogen bonded form is planar, possesses one relatively normal hydrogen bond, and has the lowest energy 3A' and 1A' states that are essentially degenerate. The 1A" and 3A" excited states produced by rotation of the unpaired OH electron into the molecular plane are very slightly bound.

Jackels, C. F.↗
NASA NTRS1986

An ab initio investigation of possible intermediates in the reaction of the hydroxyl and hydroperoxyl radicals

Ab initio quantum chemical techniques have been used to investigate covalently-bonded and hydrogen-bonded species that may be important intermediates in the reaction of hydroxyl and hydroperoxyl radicals. Stable structures of both types were identified. Basic sets of polarized double-zeta quality and large scale configuration interaction wave functions have been utilized. Based upon electronic energies, the covalently-bonded HOOOH species is found to be 26.4 kcal/mol more stable than the OH and HO2 radicals. Similarly, the hydrogen-bonded HO-HO2 species is found to have an electronic energy 4.7 kcal/mol below that of the component radicals, after correction is made for the basis set superposition error. The hydrogen-bonded form is found to be planar, to possess one relatively 'normal' hydrogen bond, and to have lowest energy 3A-prime and 1A-prime states that are essentially degenerate. The 1A-double prime and 3A-double prime excited states produced by rotation of the unpaired OH electron into the molecular plane are found to be very slightly bound.

Jackels, C. F.↗
NASA NTRS1987

Pumping the stellar hydroxyl maser

IRAS far-IR flux data for 163 OH maser stars were analyzed to quantify the contributions 35 and 53 microns inversions make to pumping of the hydroxyl maser. The 35 microns transition is from the 3,3 ground state to the 1,5 rotationally excited level and subsequent decay; the 53 microns transition is a change from the ground state to the 1,3 excited level and relaxation. The stars examined included Mira, short period semi-regular and long-period semi-regular variables. Both transition lines had rough parity in contributing to the approximately 8 percent pumping efficiency at 1612 MHz. However, the individual contributions of the lines could not be determined for the stellar population studied.

Dickinson, Dale F.↗
NASA NTRS1988

Vertical column abundance measurements of atmospheric hydroxyl from 26 deg, 40 deg, and 65 deg N

The vertical column abundance of atmospheric hydroxyl was measured with Pepsios spectrometers from Boca Raton, Florida (26.4 N); Fritz Peak, Colorado (40 deg N); and Poker Flat, Alaska (65 deg N). The data show a global solar zenith angle dependence for the OH abundances, with the general features common in measurements from all three locations since 1980. However, while theoretical models agree well with the pre-1980 abundances, the post-1980 data do not. It appears that a significant change in the atmospheric photochemistry needs to be introduced.

Burnett, Clyde R.↗
NASA NTRS1989

Periodic behaviors in the observed vertical column abundances of atmospheric hydroxyl

The data base for the vertical column abundance of atmospheric hydroxyl (OH) for Fritz Peak Observatory, Colorado (40 N, 105 W), now extends from 1976 through 1988 and is composed of 8849 independent data sets, averaging about 15 percent uncertainty and 20-minute time resolution each. The dominant solar zenith angle (chi) dependence of the OH abundance is characterized by an empirical curve, N(88), which has been updated from N(82) to include all valid data from 1980 through 1988. The chi-dependence of the OH abundance has been, to a first order, removed from the data base by a normalization procedure in which each data point is divided by the N(88,AM) value for the corresponding solar zenith angle. The resulting normalized OH values may then be examined for other systematic effects, particularly for periodic variations. Observations have also been made at Boca Raton, Florida (26 N, 80 W) and at Truk, Federated States of Micronesia (7 N, 152 E). These data bases are much less extensive and, as such, are less amenable to analysis for periodic behaviors. Some comparisons with the Colorado data may be made, however.

Burnett, Elizabeth Beaver↗
NASA NTRS1989

Spectroscopic study of combustion diagnostics on hydroxyl radicals

Experimental observations of propane/air flames have been carried out. Measurements of hydroxyl (OH) radical concentration have been made using resonance line absorption techniques. A microwave-pumped low pressure discharge in argon and water vapor is employed to produce strong OH radical band radiation in the 308 nm region. This radiation is transmitted through the plume and absorption data is taken at various radial positions using an optical multichannel analyzer. This absorption data is used to compute OH number density using a model for the absorption band characteristics as a function of temperature based on an atlas of line strengths. A numerical computation of flow fields, temperature profile, OH number density and water vapor mass fraction profiles was carried out by using a technique of computational fluid dynamics (CFD). The results of CFD computation are compared with experimental observation with a good agreement.

Eskridge, Richard↗
NASA NTRS1989

A characterization study of a hydroxylated polycrystalline tin oxide surface

In this study Auger electron spectroscopy, electron spectroscopy for chemical analysis (ESCA) and electron-stimulated desorption (ESD) have been used to examine a polycrystalline tin oxide surface before and after annealing in vacuum at 500 C. Features due to surface hydroxyl groups are present in both the ESCA and ESD spectra, and ESD shows that several chemical states of hydrogen are present. Annealing at 500 C causes a large reduction in the surface hydrogen concentration but not complete removal.

Hoflund, Gar B.↗
NASA NTRS1989

The mixing ratio of the stratospheric hydroxyl radical from far infrared emission measurements

Far infrared emission spectra of the stratosphere, measured with a 0.0033/cm resolution Fourier transform spectrometer using a limb scanning method, are analyzed in order to retrieve the vertical distribution of the hydroxyl radical (OH). The observations cover a time interval between 1300 and 2300 hours, showing a pronounced time decrease of the OH signals. Vertical profiles are obtained for the afternoon and sunset periods. An upper limit is derived from the small signals present in the night measurements. Three different methods of analysis have been applied to the same data set, and the results provided the basis for a critical discussion of the error sources. The results are compared with theoretical predictions and with the results of other experiments.

Carli, Bruno↗
NASA NTRS1990

Saturated fluorescence measurements of the hydroxyl radical in laminar high-pressure flames

The efficacy of laser saturated fluorescence (LSF) for OH concentration measurements in high pressure flames was studied theoretically and experimentally. Using a numerical model describing the interaction of hydroxyl with nonuniform laser excitation, the effect of pressure on the validity of the balanced cross-rate model was studied along with the sensitivity of the depopulation of the laser-coupled levels to the ratio of rate coefficients describing: (1) electronic quenching to (sup 2) Sigma (+) (v double prime greater than 0), and (2) vibrational relaxation from v double prime greater than 0 to v double prime = 0. At sufficiently high pressures and near-saturated conditions, the total population of the laser-coupled levels reaches an asymptotic value, which is insensitive to the degree of saturation. When the ratio of electronic quenching to vibrational relaxation is small and the rate of coefficients for rotational transfer in the ground and excited electronic states are nearly the same, the balanced cross-rate model remains a good approximation for all pressures. When the above ratio is large, depopulation of the laser-coupled levels becomes significant at high pressures, and thus the balanced cross-rate model no longer holds. Under these conditions, however, knowledge of the depletion of the laser-coupled levels can be used to correct the model. A combustion facility for operation up to 20 atm was developed to allow LSF measurements of OH in high pressure flames. Using this facility, partial saturation in laminar high pressure (less than or equal to 12.3 atm) C2H6/O2/N2 flames was achieved. To evaluate the limits of the balanced cross-rate model, absorption and calibrated LSF measurements at 3.1 and 6.1 atm were compared. The fluorescence voltages were calibrated with absorption measurements in an atmospheric flame and corrected for their finite sensitivity to quenching with: (1) estimated quenching rate coefficients, and (2) an in situ measurement from a technique employing two fluorescence detection geometries.

Carter, Campbell D.↗
NASA NTRS1990

Spectroscopic study of combustion diagnostics on hydroxyl radicals

Experimental observations of propane-air flames were performed. Measurements of hydroxyl (OH) radical concentration were made using resonance line absorption techniques. A microwave-pumped low pressure discharge in argon and water vapor is employed to produce strong OH radical band radiation in the 308 nm region. This radiation is transmitted through the plume and absorption data are taken at various radical positions using an optical multichannel analyzer. This absorption data is used to compute OH number density using a model for the absorption band characteristics as a function of temperature based on an atlas of line strengths. A numerical computation of flow fields, temperature profile and OH number density is carried out by using a technique of computational fluid dynamics (CFD). The results of CFD computation are good compared with experimental observation with a good agreement.

Hung, R. J.↗
NASA NTRS1990

Third-generation FAGE instrument for tropospheric hydroxyl radical measurement

A single-stage, frequency-doubled, copper vapor laser-pumped dye laser has been constructed to be used in the measurement of atmospheric hydroxyl radical concentrations. A new photon counting instrument is used for HO fluorescence detection. Theoretical and experimental studies of instrument performance show better sensitivities and reduced photolytic interferences than have been possible with previous systems based upon Nd:YAG pumping.

Chan, C. Y.↗
NASA NTRS1990

Carbon kinetic isotope effect in the oxidation of methane by the hydroxyl radical

The reaction of the hydroxyl radical (HO) with the stable carbon isotopes of methane has been studied as a function of temperature from 273 to 353 K. The measued ratio of the rate coefficients for reaction with (C-12)H4 relative to (C-13)H4 (k12/k13) was 1.0054 (+ or - 0.0009 at the 95 percent confidence interval), independent of temperature within the precision of the measurement, over the range studied. The precision of the present value is much improved over that of previous studies, and this result provides important constraints on the current understanding of the cycling of methane through the atmosphere through the use of carbon isotope measurements.

Cantrell, Christopher A.↗
NASA NTRS1990

Tropospheric reactions of the haloalkyl radicals formed from hydroxyl radical reaction with a series of alternative fluorocarbons

In the present assessment, the hydrogen containing halocarbons being considered as alternatives to the the presently used chlorofluorocarbons are the hydrochlorofluorocarbons (HCFCs) 123 (CF3CHCl2), 141b (CFCl2CH3), 142b (CF2ClCH3), 22 (CHF2Cl) and 124 (CF3CHFCl) and the hydrofluorocarbons (HFCs) 134a (CF3CH2F), 152a (CHF2CH3) and 125 (CF3CHF2). All of these HCFCs and HFCs will react with the hydroxyl (OH) radical in the troposphere, giving rise to haloalkyl radicals which then undergo a complex series of reactions in the troposphere. These reactions of the haloalkyl radicals formed from the initial OH radical reactions with the HCFCs and HFCs under tropospheric conditions are the focus here.

Atkinson, Roger↗
NASA NTRS1993

Far-Infrared Spectrometer Measures Stratospheric Hydroxyl

Far Infrared Limb Observing Spectrometer is balloon-borne instrument measuring far-infrared emission from limb of atmosphere. Operates in two spectral channels in wave-number range of 101 to 118 cm(to the negative 1st power). Range contains spectral lines of several molecules and radicals of current scientific interest. Instrument designed primarily to obtain data on distribution of hydroxyl radicals, which play central role in chemistry of ozone in stratosphere. Measurements contribute to understanding of "ozone hole" in stratosphere.

Peterson, Dean B.↗