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At least 199 records · Page 11

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NASA NTRS1989

Ozone precursors and ozone photochemistry over eastern North Pacific during the spring of 1984 based on the NASA GTE/CITE 1 airborne observations

Simultaneous high-resolution measurements of O3, NO, CO, dew point temperature, and UV flux obtained during the NASA Global Tropospheric Experiment Chemical Instrumentation Test and Evaluation (GTE/CITE 1) spring 1984 airborne field exercise over the eastern North Pacific Ocean are analyzed. Mid-tropospheric CO, O3, and NO mixing ratios averaged about 120 parts per billion by volume (ppbv), 50 ppbv, and 10 parts per trillion by volume (pptv), respectively. Statistical analysis of the high-resolution data indicates the existence of two ozone sources, one related to the downward transport of ozone-rich air from the upper troposphere and stratosphere, and the other to the transport of ozone-rich air from the continents. Modeling calculations based on these average levels imply that, from the surface to about 8 km, photochemical reactions probably supplied a net sink of ozone to the region overlying the eastern North Pacific Ocean during the sampling period. However, because the NO levels measured during the flights were frequently at or near the detection limit of the instruments and because the results are very sensitive to the absolute NO levels and their temporal variability, the conclusion must be considered provisional.

Chameides, W. L.↗

NASA NTRS1989

Stratospheric aerosols from CH4 photochemistry on Neptune

A combined photochemical-condensation model has been used to study hydrocarbon ices produced from CH4 photolysis in the stratosphere of Neptune. A total stratospheric haze production rate of 4.2 x 10 to the -15th g/sq cm/s. The total production rate is insensitive to within a factor of two to order of magnitude changes in the eddy diffusion coefficient and methane mixing ratio, which is within the present estimate of uncertainty for this number. The condensation temperatures are 97 K for C4H2, 71 K for C2H2, and 64 K for C2H6. Voyager 2 images of Neptune will be able to confirm the presence of stratospheric aerosols and provide constraints on their production rate and location.

Romani, Paul N.↗

NASA NTRS1990

Novel laser gain and time-resolved FTIR studies of photochemistry

Several techniques are discussed which can be used to explore laboratory photochemical processes and kinetics relevant to planetary atmospheres; these include time-resolved laser gain-versus-absorption spectroscopy and time-resolved Fourier transform infrared (FTIR) emission studies. The laser gain-versus-absorption method employed tunable diode and F-center lasers to determine the yields of excited photofragments and their kinetics. The time-resolved FTIR technique synchronizes the sweep of a commercial FTIR with a pulsed source of light to obtain emission spectra of novel transient species in the infrared. These methods are presently being employed to investigate molecular photodissociation, the yields of excited states of fragments, their subsequent reaction kinetics, Doppler velocity distributions, and velocity-changing collisions of translationally fast atoms. Such techniques may be employed in future investigations of planetary atmospheres, for example to study polycyclic aromatic hydrocarbons related to cometary emissions, to analyze acetylene decomposition products and reactions, and to determine spectral features in the near infrared and infrared wavelength regions for planetary molecules and clusters.

Leone, Stephen R.↗

NASA NTRS1990

UV and VUV spectroscopy and photochemistry of small molecules in a supersonic jet

UV and VUV absorption and emission spectroscopy is used to probe jet cooled molecules, free radicals, and clusters in the gas phase. Due to efficient cooling inhomogeneous effects on spectral line widths are eliminated. Therefore from these spectra, both structural and dynamical information is obtained. The photoproducts of these reactions are probed by resonance enhanced multiphoton ionization.

Ruehl, E.↗

NASA NTRS1989

Photochemistry of the atmosphere of Uranus

A detailed one-dimensional photochemical model incorporating vertical transport by eddy and molecular diffusion is used to study the importance of chemical and physical processes that control the hydrocarbon abundances in the stratosphere of Uranus. The study includes updated photochemical reaction rates and photolysis branching ratios; explicit calculation of the condensation rate of condensing species; and appropriate boundary conditions at the tropopause. It is found that the basic photochemical process generally produces low net conversion efficiencies of methane to higher hydrocarbons. However, even with these low efficiencies, the total condensation rate, which represents the net rate of conversion of methane to hydrocarbons, is roughly 2 x 10 to the -16th g/cm sec, in agreement with the upper range of the low condensation rate for the production of the stratospheric aerosol layer as determined by Pollack et al. (1987). Furthermore, a range of vertical transport rates is required to separately match the observational constraints on hydrocarbon abundances. The solar reflection data refer to the sunlit polar region of Uranus and require an eddy diffusion coefficient of K approx. = 50 sq cm/sec for globally averaged insolation or K approx = 1500 (Nh/N) exp 1/2 for overhead sun. The Voyager 2 Utraviolet Spectrometer solar occultation data refer to the equatorial regions, thus implying a large latitudinal gradient in stratospheric hydrocarbon abundance.

Summers, Michael E.↗

NASA NTRS1989

Photochemistry of CO and H2O - Analysis of laboratory experiments and applications to the prebiotic earth's atmosphere

The role photochemical reactions in the early earth's atmosphere played in the prebiotic synthesis of simple organic molecules was examined, extending an earlier calculation of formaldehyde production rates to more reduced carbon species, such as methanol, methane, and acetaldehyde. The experimental results of Bar-Nun and Chang (1983) are simulated as an aid in the construction of the photochemical scheme and as a way of validating the model. The results indicate that some fraction of CO2 and H2 present in the primitive atmosphere could have been converted to simple organic molecules. The exact amount is dependent on the partial pressure of CO2 and H2 in the atmosphere and on what assumptions are made concerning the shape of the absorption spectra of CO2 and H2O.

Wen, Jun-Shan↗

NASA NTRS1990

Uranus photochemistry and prospects for Voyager 2 at Neptune

CH4 is the only photochemically active constituent in the atmospheres of Uranus and Neptune. NH3, H2O and H2S are all removed by condensation at pressures greater than 1.5 bars. Although the bulk mole fraction (about 2 percent) of CH4 is 20-30 times its solar value on both planets, it drops to its saturation limit (about 0.0001) at the Uranus tropopause, but remains high (about 2 percent) at the Neptune tropopause. This results in much greater mixing ratios of the product hydrocarbons in the stratosphere of Neptune. On both planets, the photolysis products of CH4 undergo condensation near the tropopause and the upper stratosphere. Voyager observations of the hydrocarbons at Uranus and those planned at Neptune are discussed, along with their implications for upper-atmospheric physics and thermochemistry.

Atreya, S. K.↗

NASA NTRS1988

The photochemistry of planetary atmospheres

Recent theoretical and observational investigations of photochemical processes in the atmospheres of the planets and their satellites are reviewed. Particular attention is given to the CO2-dominated atmospheres of Mars and Venus, the hydrogen-dominated atmospheres of the Jovian planets, the SO2 atmosphere of Io, and the massive atmospheres of Titan and Triton. The principal reaction paths involved are listed and briefly characterized, and numerical data on atmospheric compositions are given in tables.

Dalgarno, A.↗

NASA NTRS1990

The seasonal variation of water vapor and ozone in the upper mesosphere - Implications for vertical transport and ozone photochemistry

This paper reviews the data base supplied by ground-based microwave measurements of water vapor in the mesosphere obtained in three separate experiments over an eight-year period. These measurements indicate that the seasonal variation of water vapor in the mesosphere is dominated by an annual component with low values in winter and high values in summer, suggesting that the seasonal variation of water vapor in the mesosphere (below 80 km) is controlled by advective rather than diffusive processes. Both the seasonal variation and the absolute magnitude of the water vapor mixing ratios obtained in microwave measurements were corroborated by measurements obtained in the Spacelab GRILLE and ATMOS experiments, and were found to be consistent with several recent mesospheric dynamics studies.

Bevilacqua, Richard M.↗

NASA NTRS1990

The polar stratospheric cloud event of January 24. II - Photochemistry

During the 1988/89 Airborne Arctic Stratospheric Expedition (AASE), observations of the chemical composition, aerosol characteristics and atmospheric state were obtained from two aircraft, a NASA ER-2 and a DC-8. This paper presents a diagnosis of observations obtained using the ER-2 on January 24, 1989, using a Lagrangian coupled microphysical-photochemical model. The high chlorine monoxide mixing ratios observed from the ER-2 on the afternoon of January 24, 1989 are interpreted as a result of in situ heterogeneous release of reactive chlorine from the reservoirs HCl and CIONO2 on type-1 polar stratospheric cloud particles observed to be present at that time. This essential element in theories of polar ozone depletion has never before been observed directly in the stratosphere.

Jones, R. L.↗

NASA NTRS1990

The photochemistry of methane in the atmosphere of Triton

The model of Summers and Strobel (1989) for photochemical reactions in the Uranus atmosphere was modified and used for quantitative calculations of methane in the atmosphere of Triton. The principal adjustable parameters in the new model are the surface CH4 concentrations and the vigor of vertical mixing in Triton's lower atmosphere. It is shown the rate of methane photolysis that was calculated is sufficient to generate a smog of condensed C2H2, C2H4, C2H6, and C4H2 particles in the lowest 30 km of Triton's atmosphere, with an optical depth consistent with the Voyager imaging results.

Strobel, Darrell F.↗

NASA NTRS1989

New insights in the photochemistry of grain mantles: The identification of the 4.62 and 6.87 micron bands

The mid-IR spectral region of molecular clouds is known to show the fingerprints of molecules frozen in the icy mantles of the interstellar grains. To study the complex chemical and physical interactions on the ice mantles accreted on grains in molecular clouds numerous UV irradiation and diffusion experiments were performed. The irradiation of binary ices was studied. Using isotopic labelling on NH3/CO and NH3/O2 ices numerous compounds were identified, of which OCN(-), NO2(-), NO3(-), and NH4(+) ions reveal a new type of chemical reactions. It appeared that these compounds were formed by proton transfer reactions induced by the interaction between an acid (HNCO, HNO2, HNO3) and a base (NH3) through a hydrogen bond. This mechanism was confirmed by a study of photolyzed diluted argon mixtures. The main astrophysically relevant data from the overall study are presented. The 4.62 micron band in W33A can be reproduced with NH3/CO containing irradiated ices and was identified with OCN(-). The 6.87 micron band in W33A and other photostellar objects is reproduced with NH3/O2 containing ices and is identified with NH4(+).

Grim, Ruud↗

NASA NTRS1989

The UV photochemistry of C2N2

The absorption, emission, and photodissociation yield spectra of C2N2 were measured in the 220 and 210 nm region near the 4(0)1 and 1(0)1 4(0)1 bands of the A 1 sigma + from the X 1 sigma + system. The emission spectrum showed very few lines which appeared in the absorption spectrum. Moreover, the emission had 660 ns lifetime and, at 210 nm a very large electronic emission quenching rate. Laser induced fluorescence was used to measure the relative yield of CN radicals as a function of photolysis wavelength. This spectrum seemed to follow the absorption spectrum below the dissociation threshold. Energy in the CN fragments appeared to be statistically distributed.

Halpern, Joshua B.↗

NASA NTRS1991

Vertical mixing and methane photochemistry in the atmosphere of Uranus: Analysis of Voyager UVS occultation experiments

Extensive capabilities were developed in the analysis of ultraviolet spectrometer (UVS) absorptive lightcurves. The application of these capabilities to the Voyager UVS data sets from Uranus and Neptune has provided significant findings regarding the stratospheres of these planets. In particular, the direct comparison between photochemical models and UVS measurements accomplished by these efforts is unique, and it helps to guarantee that the information returned by the Voyager 2 spacecraft is being used to the fullest extent possible.

Bishop, James↗

NASA NTRS1990

Are there interactions of iodine and sulfur species in marine air photochemistry?

The effects of dimethyl sulfide (DMS) and methyl iodide (MI) emissions are analyzed using a two-dimensional photochemical model of a marine tropical tropospheric synoptic system. The model traces the atmospheric transformation cycles of the emissions to aerosols. The study is focused on remote tropical ocean regions and includes simulations of the spatial and diurnal variations of various iodine and sulfur species, and the species OH, HO2, and H2O2. One line of analysis leads to the conclusion that the reaction IO + DMS yields DMSO + I may play a significant role in destroying DMS if it proceeds at the published fast rate. Alternative lines of analyses are presented.

Chatfield, Robert B.↗

NASA NTRS1991

Troposphere-stratosphere interactions in a one-dimensional model of Jovian photochemistry

The case of a chemically unreactive species flowing downward through the stratosphere and troposphere with a constant flux is presently treated by a one-dimensional Jovian atmosphere model which encompasses the coupling between a rapidly mixed troposphere and a stagnant stratosphere, so that the contrast between the peak stratosphere and tropopause concentrations is reflective of the variation between the lower stratosphere and upper troposphere eddy diffusion coefficients. Numerical simulations of unreactive CO and C2H6 species indicate that upper troposphere abundances may possess a substantial photochemical contribution. The implications of these modeling results for higher spectral resolution observations are noted.

Landry, Bridget↗

NASA NTRS1991

A test of odd-oxygen photochemistry using Spacelab 3 atmospheric trace molecule spectroscopy observations

The ozone profile calculated using a 1D time-dependent photochemical model, with recommended absorption cross sections and reaction rate constants, is systematically less than Spacelab 3 (May 1985) atmospheric trace molecule spectroscopy (ATMOS) observations at sunset, 30 deg N latitude, throughout the upper stratosphere and mesosphere. Model results are about 9 percent smaller than the nominal ATMOS O3 value at 40 km and 50 percent less at 76 km. Given the uncertainties associated with the ATMOS profile, the model 'deficit' may be as large as 15 percent at 36 km, increasing to about 70 percent at 76 km. A similar model O3 deficit exists at sunrise, 47 deg S latitude, in the stratosphere: nominal differences of not more than 25 percent, increasing to not more than 45 percent when the ATMOS uncertainties are considered. Model results closely approximate ATMOS observations in both the upper stratosphere and mesosphere upon enhancing odd-oxygen production by increasing the O2 Schumann-Runge band and Herzberg-continuum cross section values used in the calculations.

Allen, Mark↗

NASA NTRS1991

Implications of C2H photochemistry on the modeling of C2 distributions in comets

Laboratory studies of the secondary photolysis of the C2H radical are summarized and used to explain some discrepancies between models of C2 emission in comets. These studies show that several states of the C2 radicals produced in the photolysis of C2H2 at 193 nm have bimodal rotational distributions when plotted as a Boltzmann diagram. They also establish that the C2 radicals are formed with varying degrees of vibrational excitation, so that if they are formed in a similar manner in comets, the C2 radicals must start out with this initial vibrational excitation.

Jackson, William M.↗