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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

Iodine - Its possible role in tropospheric photochemistry

A detailed study of the photochemistry of iodine and its oxides indicates that iodine species may play an important role in the tropospheric photochemical system. Methyl iodide, often observed in the marine troposphere with an average concentration of 5-10 ppt, is photolyzed and thereby produces I atoms. Chemical interactions with O3, HxOy, and NOx cause I to be converted to other inorganic compounds such as IO, HOI, IONO2, and I2. The production of these species and their subsequent recycling back to I can lead to the catalytic removal of tropospheric O3, the enhancement of the NO2/NO ratio, the destruction of HxOy free radicals, and the conversion of HO2 to OH. Ultimately, tropospheric inorganic iodine is removed by heterogeneous processes. Calculations using a numerical model to simulate tropospheric photochemistry indicate that iodine may have a strong impact upon the atmospheric O3-NOx-HxOy system. The magnitude of these effects is dependent upon the value of several uncertain rate constants and the primary source distributions of CH3I and other organic and inorganic iodine compounds.

Chameides, W. L.↗
NASA NTRS1981

Effects of multiple scattering and surface albedo on the photochemistry of the troposphere

The effect of treatment of incoming solar radiation on the photochemistry of the troposphere is discussed. A one dimensional photochemical model of the troposphere containing the species of the nitrogen, oxygen, carbon, hydrogen, and sulfur families was developed. The vertical flux is simulated by use of the parameterized eddy diffusion coefficients. The photochemical model is coupled to a radiative transfer model that calculates the radiation field due to the incoming solar radiation which initiates much of the photochemistry of the troposphere. Vertical profiles of tropospheric species were compared with the Leighton approximation, radiative transfer, matrix inversion model. The radiative transfer code includes the effects of multiple scattering due to molecules and aerosols, pure absorption, and surface albedo on the transfer of incoming solar radiation. It is indicated that significant differences exist for several key photolysis frequencies and species number density profiles between the Leighton approximation and the profiles generated with, radiative transfer, matrix inversion technique. Most species show enhanced vertical profiles when the more realistic treatment of the incoming solar radiation field is included

Augustsson, T. R.↗
NASA NTRS1981

Comets and the photochemistry of the paleoatmosphere

Ozone (O3) is a key atmospheric gas in considerations of the photochemistry/chemistry of the paleoatmosphere, chemical evolution, and the origin and evolution of life. The photochemistry/chemistry of atmospheric O3 in the paleoatmosphere is investigated using a one-dimensional photochemical model that includes the chemistry of oxygen, nitrogen, hydrogen, carbon, and chlorine gases. The role of cometary influx of H2O on the photochemistry of the paleoatmosphere is also examined. Recently, it has been suggested that the planet received a significant portion of the volatiles presently in the atmospheric/oceanic/biospheric system from cometary volatile influx. Several consequences of a cometary H2O influx on the photochemistry and structure of the paleoatmosphere are presented.

Levine, J. S.↗
NASA NTRS1982

Photochemistry of the stratosphere of Venus - Implications for atmospheric evolution

The photochemistry of the Venus stratosphere is modeled using an updated and expanded chemical scheme along with the results of recent observations and laboratory studies. Three models, with H2 mixing ratio equal to 2 x 10 to the -5th, 5 x 10 to the -7th, and 1 x 10 to the -13th, respectively, are examined. All three models are found to satisfactorily account for the observations of CO, O2, O2(1Delta), and SO2 in the stratosphere, but only the last one may be able to account for the diurnal behavior of mesospheric CO and the UV albedo. Oxygen, derived from CO2 photolysis, is mainly consumed by CO2 recombination and oxidation of SO2 to H2SO4. The photolysis of HCl in the upper stratosphere provides a major source of odd hydrogen and free chlorine radicals, essential for the catalytic oxidation of CO. Oxidation of SO2 by O occurs in the lower stratosphere. The modeling reveals a number of interesting similarities, previously unsuspected between the chemistry of the stratosphere of Venus and that of the earth; photochemistry may have played a major role in the evolution of the atmosphere.

Yung, Y. L.↗
NASA NTRS1983

Photochemistry of acetylene at 1849 A

It is pointed out that the photochemistry of acetylene in the 1500-2000 A region at low pressure, particularly the quantum yield of C2H production and the reactions of C2H with H2 and hydrocarbons, is important in understanding the photochemistry of Jovian and Titan atmospheres. The present investigation was initiated to obtain information on these issues. The 1849 A light source used in the study was a sealed quartz tube containing a drop of Hg and 2 torr of Ar excited by a microwave generator. The lamp was attached to a Pyrex reaction cell. The amount of diacetylene produced was measured on the basis of absorption near 1650 A. Reaction mixtures of acetylene with N2, He, C2H6, or C3H8 were prepared. Attention is given to the absorption cross section, the photolysis of acetylene, and the photolysis of acetylene in the presence of other gases. It is found that the photochemical process of acetylene at 1849 A may represent that of acetylene in the Titan atmosphere.

Okabe, H.↗
NASA NTRS1983

Phosphine photochemistry in Saturn's atmosphere

The phosphine photochemistry on Saturn is studied with a 1D photochemical model. The PH3 concentration is rapidly depleted with height (scale height 3.5 km) in the upper troposphere. Formation of P, a probable precursor of P4, (a potential red chromophore in the atmosphere), is highly improbable unless the rate constant for the recombination reaction PH + H2 + M yields PH3 + M is less than 10 to the -41st cm exp 6/molecule-squared sec. Coupling of PH3 and hydrocarbon photochemistry, specifically the C2H2 catalyzed photodissociation of CH, is important. Column production rates of the organophosphorus compounds CH3PH2 and HCP of 3 x 10 to the 8th/sq cm sec are predicted, with potentially observable column densities of greater than 1 x 10 to the 17th/sq cm.

Kaye, J. A.↗
NASA NTRS1985

The photochemistry of biogenic gases in the early and present atmosphere

The distribution of gases in the prebiologial paleoatmosphere is investigated using photochemical models. A chart of the photochemical and chemical reactions and reaction rates for CH4, NH3, H2S, N2O, and CO atmospheric gases is given. Mixing ratios and surface mixing ratios for CH4, NH3, CO, and N2O are obtained using thermodynamic equilibrium calculations; an increase in CH4 and N2O is observed. The reactions, which explain the photochemistry of the gases studied, are presented. The sources of these gases and their concentration with regards to altitude are examined. Graphs of the vertical distribution of CH4, NH3, H2S, CO, O2, and N2O in prebiological paleoatmosphere are provided. The data reveals the presence of only N2, CO2, and N2O in the early atmosphere; with the evolution of life, sources of atmospheric gases increased and their influence on the photochemistry of the troposphere and stratosphere increased.

Levine, J. S.↗
NASA NTRS1985

The photochemistry of methane and carbon monoxide in the troposphere in 1950 and 1985

The roughly 1 percent/year increase in tropospheric methane and roughly 2 percent/year increase in tropospheric carbon monoxide deduced from recent analyses of ground-based solar infrared spectra recorded in 1950 and 1951 have very important implications for the photochemistry and chemistry of the troposphere. Photochemical calculations indicate that as a result of the increase of methane and carbon monoxide since 1950-51, levels of the hydroxyl radical, the key species in the photochemistry of the troposphere, may have decreased by about 25 percent.

Levine, J. S.↗
NASA NTRS1985

The photochemistry of the early atmosphere

The composition of the earth's present atmosphere is described. The formation of the earth from the coalescence and accretion of the refractory elements of the solar nebula is examined. Two possible compositions of the prebiological paleoatmosphere, which are a reducing atmosphere of CH4, NH3, and H2 or a mildly reducing atmosphere of H2O, CO2, and N2, and their photochemistry are analyzed. General photochemical and chemical processes are reviewed. The use of the coupled continuity-transport equation to calculate the vertical distribution of each species is discussed. A study of the photochemical process of CH4 and NH3 reveals that the reducing atmosphere could not possibly exist. An analysis of the photochemistry and chemistry of the H2O, CO2, and N2 atmosphere reveals that the photodissociation of H2O and CO2 results in a prebiotic source of O2, H2CO, and HCN, which are the components for the evolution of photosynthetic organisms and a strongly oxidizing atmosphere. The reactions which produce O2 and H2CO from H2O and CO2, and the relation between H2O and CO2 concentrations and O2 levels are investigated. The formation of O3 photochemically from O2 is explained.

Levine, J. S.↗
NASA NTRS1988

Methane photochemistry and methane production on Neptune

The Neptune stratosphere's methane photochemistry is presently studied by means of a numerical model in which the observed mixing ratio of methane prompts photolysis near the CH4 homopause. Haze generation by methane photochemistry has its basis in the formation of hydrocarbon ices and polyacetylenes; the hazes can furnish the requisite aerosol haze at the appropriate pressure levels required by observations of Neptune in the visible and near-IR. Comparisons of model predictions with Uranus data indicate a lower ratio of polyacetylene production to hydrocarbon ice, as well as a lower likelihood of UV postprocessing of the acetylene ice to polymers on Neptune, compared to Uranus.

Romani, P. N.↗
NASA NTRS1989

Examination of stratospheric ozone photochemistry in light of recent data

The consistency of stratospheric ozone photochemistry is examined using data from the Atmospheric Trace Molecule Spectroscopy (ATMOS) and LIMS experiments. The ATMOS experiment measured vertical profiles of important trace constituents and temperature in the stratosphere during 1985. These observations have been used to constrain the levels of odd nitrogen and odd chlorine in a photochemical model. This model yields O3 mixing ratios that are in good agreement with the observations. The deviation in ozone is less than 20 percent except near 52 km. The updated model has also been used in conjunction with the LIMS data to simulate the stratospheric photochemistry corresponding to the 1979 time period.

Natarajan, Murali↗
NASA NTRS1990

Laboratory measurements and methane photochemistry modeling

Methane is photolyzed by the solar UV in the stratosphere of Saturn. Subsequent photochemistry leads to the production of acetylene (C2H2) and diacetylene (C4H2). These species are produced where it is relatively warm (T is greater than or equal to 140 K), but the tropopause temperature of Saturn (approximately 80 K) is low enough that these two species may freeze out to their respective ices. Numerical models which include both photochemistry and condensation loss make predictions about the mixing ratios of these species and haze production rates. These models are dependent upon knowing reaction pathways and their associated kinetic reaction rate constants and vapor pressures. How uncertainties in the chemistry and improvements in the vapor pressures affect model predictions for Saturn are discussed.

Romani, P. N.↗
NASA NTRS1994

Ultraviolet photochemistry of cyanoacetylene: Application to Titan

Cyanoacetylene is believed to have had a central role in the formation of the pyrimidines essential for RNA synthesis leading to the origin of life on Earth. Cyanoacetylene has also been detected on Titan, Saturn's largest moon, and the only moon in the solar system that possesses a dense atmosphere. It is generally accepted that photochemistry plays a major role in the formation of the complex organic molecules and aerosols found in Titan's atmosphere. Because of its long wavelength absorption and low dissociation threshold it is expected that cyanoacetylene is an important part of these photochemical processes. Since cyanoacetylene would also have been subject to ultraviolet light in the atmosphere of early Earth, an investigation of cyanoacetylene photochemistry on Titan might lead to a better understanding of both the photochemical reactions occurring on primitive earth and the processes of chemical evolution as they occur in planetary atmospheres. The effects of irradiation wavelength, mixing with Titan's atmospheric gases, reducing the temperature and lowering cyanoacetylene partial pressures on product formation and polymer composition have been determined with the ultimate goal of understanding the chemical transformations taking place in Titan's atmosphere.

Clarke, D. W.↗
NASA NTRS1997

Lyman Alpha Photochemistry in the Solar Nebula

The purpose of the project "Lyman Alpha Photochemistry in the Solar Nebula" was to model photochemistry in the primitive solar nebula and the early solar systems. As part of the modeling, it was necessary to model the composition of the gas and dust accreted by the solar nebula. This final report contains a list of publications where the results of this project have been published.

Fegley, Bruce, Jr.↗
NASA NTRS1997

Atmospheric Transport and Photochemistry of Ozone Over Central Southern Africa During the Southern Africa Fire-Atmosphere Research Initiative

Vertically integrated back and forward trajectories for the 300-200, 700-500 and surface-800 hPa levels are calculated using Pretoria as point of origin for the Southern Africa Fire-Atmosphere Research Initiative (SAFARI) period September-October 1992. The transport fields are then combined to show both horizontal and vertical transport of air to and from Pretoria at the different levels. Air transport patterns in the vertical are linked to the occurrence of absolutely stable layers which are also evident in the 16 ozonesonde profiles recorded at Pretoria during SAFARI. The coherence of the stratification based on dynamical and ozone analysis permits the use of mean ozone profiles with air volume fluxes to interpret the ozone in terms of photochemistry and transport within stable layers. Extensive recirculation across the meridional plane at Pretoria implies that advection of ozone is slow and that photochemistry is responsible for the observed vertical structure over central southern Africa in September and October 1992. Requisite ozone formation rates are supported by model analysis of ozone and ozone precursors measured from SAFARI and Transport and Atmospheric Research Chemistry near the Equator-Atlantic aircraft.

Tyson, P. D.↗
NASA NTRS1999

[A Study of Data From the Photochemistry of Ozone Loss in the Arctic Region In Summer (POLARIS) Mission]

The Photochemistry of Ozone Loss in the Arctic Region In Summer (POLARIS) mission was designed to investigate the natural summer decrease of stratospheric ozone levels. Both polar regions have large and distinct annual cycles of ozone column amounts. In northern spring, the average level is over 450 Dobson units (DU), decreasing to less than 275 DU by September. In order to cover this period of ozone decrease, POLARIS was conducted in three deployment phases from Fairbanks, Alaska, (650N) during the summer of 1997. The principal measurement platforms were the NASA ER-2 high-altitude aircraft and stratospheric balloons. Additional measurements were provided by ground-based instruments, sondes, and satellites. POLARIS observations included ozone, meteorological variables, particles, long-lived chemicals, and short-lived radicals. During the field deployments, several modeling and theoretical groups participated in flight planning and data evaluation activities. The interpretive studies in this Special Section of the Journal of Geophysical Research are a first comprehensive examination of the POLARIS data set, addressing stratospheric ozone abundances and its changes; the role of aerosols; details of the photochemistry of reactive species; transport of stratospheric air and the correlations of long-lived species; and measurement intercomparisons.

Newman, Paul A.↗
NASA NTRS1999

Photochemistry of Oxygen Compounds in Neptune's Stratosphere

ISO SWS observations of H2O and CO2 on Neptune (Feuchtgruber et al. 1997, Nature 389, 159) coupled with ground based millimeter observations of CO (Marten et al., 1993, Ap. J. 406 285) provide strong constraints on the photochemistry of these compounds in Neptune's stratosphere. Additional constraints on the photochemistry and vertical mixing come from the rich suite of hydrocarbons observed by ISO: CH4, C2H2, C2H6 (Bezard, 1998, Ann. Geophysicae 16, Sup. III C1037), CH3 (Bezard, et al. Ap. J. 515, 868), and C2H4 (Encrenaz et al. this DPS). We will use a one-dimensional global average photochemical model to analyze these compounds. In particular, we will better constrain the estimated external flux of H2O to Neptune's stratosphere given in Feuchtgruber et al., which is important in understanding the source of the observed stratospheric CO2. Kingdoms will come and go, the relentless march of time will continue, all will be explained.

Romani, P. N.↗
NASA NTRS1999

Photochemistry of Pluto's Atmosphere

This work include studies of two problems: (1) Modeling thermal balance, structure. and escape processes in Pluto's upper atmosphere. This study has been completed in full. A new method, of analytic solution for the equation of hydrodynamic flow from in atmosphere been developed. It was found that the ultraviolet absorption by methane which was previously ignored is even more important in Pluto's thermal balance than the extreme ultraviolet absorption by nitrogen. Two basic models of the lower atmosphere have been suggested, with a tropopause and a planetary surface at the bottom of the stellar occultation lightcurve, respectively, Vertical profiles, of temperature, density, gas velocity, and the CH4 mixing ratio have been calculated for these two models at low, mean, and high solar activity (six models). We prove that Pluto' " s atmosphere is restricted to 3060-4500 km, which makes possible a close flyby of future spacecraft. Implication for Pluto's evolution have also been discussed. and (2) Modeling of Pluto's photochemistry. Based on the results of (1), we have made some changes in the basic continuity equation and in the boundary conditions which reflect a unique can of hydrodynamic escape and therefore have not been used in modeling of other planetary atmospheres. We model photochemistry of 44 neutral and 23 ion species. This work required solution of a set of 67 second-order nonlinear ordinary differential equations. Two models have been developed. Each model consists of the vertical profiles for 67 species, their escape and precipitation rates. These models predict the chemical structure and basic chemical processes in the current atmosphere and possible implication of these processes for evolution. This study has also been completed in full.

Krasnopolsky, Vladimir A.↗