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NASA NTRS1985

Measurements of concentrations of chlorofluoromethanes (CFMs) carbon dioxide and carbon isotope ratio in stratospheric and tropospheric air by grab-sampling systems

Measurements of concentrations of chlorofluoromethanes (CFMs), carbon dioxide and carbon isotope ratio in stratospheric and tropospheric air by grab-sampling systems are reported. The balloon-borne grab-sampling system has been launched from Sanriku Balloon Center three times since 1981. It consists of: (1) six sampling cylinders, (2) eight motor driven values, (3) control and monitor circuits, and (4) pressurized housing. Particular consideration is paid to the problem of contamination. Strict requirements are placed on the choice of materials and components, construction methods, cleaning techniques, vacuum integrity, and sampling procedures. An aluminum pressurized housing and a 4-m long inlet line are employed to prevent the sampling air from contamination by outgassing of sampling and control devices. The sampling is performed during the descent of the system. Vertical profiles of mixing ratios of CF2Cl2, CFCl3 and CH4 are given. Mixing ratios of CF2Cl2 and CFCl3 in the stratosphere do not show the discernible effect of the increase of those in the ground level background, and decrease with altitude. Decreasing rate of CFCl3 is larger than that of CF2Cl2. CH4 mixing ratio, on the other hand, shows diffusive equilibrium, as the photodissociation cross section of CH4 is small and concentrations of OH radical and 0(sup I D) are low.

Itoh, T.↗
NASA NTRS1985

Water vapor content in the polar atmosphere measured by Lyman-alpha/OH fluorescence method

The water vapor of the polar stratosphere possibly plays an important role in various aeronomical processes; for example, OH radical formation through photodissociation of H2O, formation of water cluster ions, radiative energy transfer in the lower stratosphere, condensation onto particulate matter, and so on. In addition to these, it has been speculated, from the viewpoint of global transport and/or budget of water vapor, that the polar stratosphere functions as an active sink. STANFORD (1973) emphasized the existence of the stratospheric Cist cloud in the polar stratosphere which brought a large loss rate of stratospheric water vapor through a so-called freeze-out of cloud particles from the stratosphere into the troposphere. However, these geophysically interesting problems unfortunately remain to be solved, owing to the lack of measurements on water vapor distribution and its temporal variation in the polar stratosphere. The water vapor content measured at Syowa Station (69.00 deg S, 39.35 deg E), Antarctica using a balloon-borne hygrometer (Lyman - alpha/OH fluorescence type) is discussed.

Iwasaka, Y.↗
NASA NTRS1986

Design and chemical synthesis of iodine-containing molecules for application to solar-pumped I* lasers

The design and chemical synthesis of new media for solar pumped iodine molecule lasers are explored. In an effort to prepare an iodo fluorocarbon compound absorbing strongly at 300 nm or above, the synthesis of perfluoro allylic iodides was investigated. These compounds furnish especially stable allylic radicals upon photodissociation. The desired red shift is anticipated in the absorption maximum could correlate with increasing radical stability. This expectation was based upon the analysis, previously reported, of the structures and absorption maxima of compounds studied earlier. A previously unknown substance was prepared, a prototypical target molecule, perfluoro-3-iodocyclopent-1-ene. It was obtained by reaction of perfluorocyclopentene with sulfur trioxide under the influence of antimony pentafluoride catalyst, followed by treatment of the resulting allylic fluorosulfonate with sodium iodide in sulfoland solvent. Preliminary data indicate that the absorption maximum for the iodo fluorocarbon is not shifted significantly to longer wavelength. It is not certain whether this result reflects an unexpected influence of the cyclic structure upon the position of the absorption maximum.

Shiner, C. S.↗
NASA NTRS1985

On the production of N(+) by energetic electrons

Calculations of the ratio of N(+) to total N2 ion production for auroral electrons which give a value of 0.16 compared to the value of 0.22 that has been assumed in a recent publication is presented. The corresponding ratio for photoelectron production is 0.05, which makes photoelectron production of N(+) negligible compared to photodissociative production. The ratio of 3914-A to total ion production is found to be 0.07 for auroral electrons and a similar 0.06 for photoelectrons. The 3371-A ratio to total N2 ion production is 0.09. This calculation also reveals that the secondary electrons in auroras, with energies less than 100 eV, produce only about one third of the total number of ions produced. Only one quarter of the N(+) ions are created by secondary electrons.

Richards, P. G.↗
NASA NTRS1985

Ozone in the free atmosphere

The present book provides a summary of the state of scientific knowledge of stratospheric and free tropospheric ozone as it exists at the beginning of 1983. Ozone photochemistry in the stratosphere is discussed, taking into account fundamental molecular properties, the absorption spectrum of ozone, photodissociation, ozone formation and destruction in the upper atmosphere, the photochemistry of odd-hydrogen, the photochemistry of odd-nitrogen, the photochemistry of odd-chlorine, and photochemistry-temperature coupling. The observed distribution of atmospheric ozone and its variations are considered along with ozone transport, ozone in the troposphere, stratospheric ozone perturbations, and climatic and biological effects. Attention is given to the techniques of observing atmospheric ozone, horizontal-vertical ozone transport and conservative quantities, measurements of tropospheric ozone, the tropospheric ozone budget, ozone models, natural ozone variations, and anthropogenic ozone perturbations.

Whitten, R. C.↗
NASA NTRS1985

An upper limit for the absorption cross section of the oxygen C 3 Delta u - a 1 Delta g transition

Frederick and Cicerone (1985) have proposed that photodissociation of O2 (a 1 Delta g) by the process O2 (a 1 Delta g) + h-nu + O2 (C 3 Delta u) to O(3 P) + O(3 P) may be a major source of odd oxygen in the upper stratosphere and mesosphere. They argued that, since the process is forbidden only by change in the spin multiplicity, it might have been a cross section intermediate between a fully allowed and a strictly forbidden transition, i.e., 10 to the -20th to 10 to the -19th sq cm near 250 nm. In order to test this proposal, absorption by O2 (a 1 Delta g) has been measured in the 190-290 nm wavelength region. No absorption above the detection limit could be observed for O2 (a 1 Delta g) concentrations of (4-7) x 10 to the 15th/cu cm. An upper limit of 8 x 10 to the -22 sq cm was calculated for the cross section.

Simonaitis, R.↗
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 NTRS1986

Origin of ultra-high-energy gamma-rays from Cygnus X-3 and related sources

Diffusive shock acceleration of ions is examined as the mechanism responsible for the ultrahigh energy (UHE) gamma ray emission observed from Cygnus X-3 and several other binary X-ray sources at energies of 10 to the 15th eV and higher. The shock acceleration can under reasonable assumptions be sufficiently short to allow acceleration of ions to energies near 10 to the 16th eV. It is proposed that the subsequent proton-proton collisions and photodissociation of He-4 can produce a flux of neutrons that escapes from the acceleration site despite high magnetic fields. These neutrons, by interacting with the binary companion, produce the observed UHE radiation.

Kazanas, D.↗
NASA NTRS1986

Two-dimensional monthly average ozone balance from limb infrared monitor of the stratosphere and stratospheric and mesospheric sounder data

For many years, atmospheric scientists have been concerned with the balance of ozone production and loss terms in the upper stratosphere. Crutzen and Schmailzl (1983) found that the ozone loss was higher than the ozone production in the upper stratosphere. In the present investigation, previous studies are used as a basis in the conduction of a two-dimensional calculation of the production and loss of ozone. The monthly and zonally averaged loss and production rates for ozone are computed using recent Nimbus 7 satellite measurements of stratospheric constituents and accepted reaction and photodissociation rates. It is found that ozone has a loss rate which is about 40-60 percent higher than the production in the photochemical region.

Jackman, C. H.↗
NASA NTRS1986

Photochemistry of methane and the formation of hydrocyanic acid (HCN) in the earth's early atmosphere

A one-dimensional photochemical model is used to analyze the photochemistries of CH4 and HCN in the primitive terrestrial atmosphere. CH4, N2, and HCN photolysis are examined. The background atmosphere and boundary conditions applied in the analysis are described. The formation of HCN as a by-product of N2 and CH4 photolysis is investigated; the effects of photodissociation and rainfall on HCN is discussed. The low and high CH4 mixing ratios and radical densities are studied.

Zahnle, K. J.↗
NASA NTRS1986

The origin of CS in comet IRAS-Araki-Alcock 1983d

It is shown that the IUE observations of CS in the atmosphere of comet IRAS-Araki-Alcock 1983d are consistent with its formation by the photodissociation of CS2 released from the nucleus. The observed scale length can be matched by a calculated scale length, which is based on the photochemical lifetime of CS2 at 1 AU and hydrodynamic models of the velocity field in the coma. A flow velocity of about 0.6 km/s is required to fit the data, which is in excellent agreement with recent calculations of the flow regime in the inner coma.

Jackson, W. M.↗
NASA NTRS1986

Observations of the diurnal variation of nitrogen dioxide in the stratosphere

Observations of NO2 from the limb infrared monitor of the stratosphere (LIMS) experiment in high-latitude summer are presented. Appropriate selection of latitude and days during the month of May yields NO2 observations obtained during the afternoon and evening at solar zenith angles ranging from about 35-110 deg. These data show that the NO2 abundances in the stratosphere become strongly dependent on the solar zenith angle for angles exceeding about 80 deg. Model calculations and other observations suggest that from about 80-95 deg this dependence probably reflects variations in the propagation of the visible radiation that photodissociates NO2. The data obtained at zenith angles greater than about 95 deg provide clear evidence for the night decay of NO2 to form N2O5, and the observed decay rate is shown to be consistent with present theory.

Solomon, S.↗
NASA NTRS1985

Cometary comae

The basis of our knowledge about the structure and composition of a comet nucleus is examined. Such knowledge is inferred from observations of the cometary atmosphere (coma). However, photodissociation, photoionization, and chemistry destroy the mother molecules evaporating from the nucleus. To extract the primary information, the chemical kinetics and the physics of the coma are modeled with a computer and the results are compared with coma observations. The physics and chemistry for a dust free coma are described taking into account energy balance, multi-fluid flow for fast atomic and molecular hydrogen and the bulk fluid, and the transition from a collision dominated inner region to the free molecular flow outer region. Special attention is paid to the molecular data requirements for the current modeld and for extended models which will include solar wind interaction and dust. Such models are an important tool in support of the Giotto mission to Halley's comet, in the analysis and interpretation of coma observations, and in the understanding of the earliest history of the solar system.

Huebner, W. F.↗
NASA NTRS1986

A long-pulse amplifier for solar-pumped iodine lasers

The characteristics of a photodissociation iodine-laser amplifier pumped with a solar-simulating radiation were studied. Under long-pulse energy extraction, an energy amplification of about three and an energy storage time of longer than 500 microseconds were observed for a one meter long, 10 mm i.d. amplifier tube. The effects of elevated temperatures resulted in little reduction of the amplifier gain. These results confirm that developing an efficient chain of oscillator-amplifiers for a high-power solar-pumped iodine laser is indeed feasible.

Hwang, I. H.↗
NASA NTRS1985

Diffuse 157-micron C II forbidden-line emission from the Galaxy

The diffuse 157.74-micron C II forbidden-line emission from the Galaxy was sampled at several longitudes near the galactic plane including complete scans across the plane at l(II) = 2.16 deg and l(II) = 7.28 deg. The observed C II forbidden-line profiles closely follow the nearby C-12O (J = 1-0) emission profiles. The C II forbidden-line emission probably arises in neutral photodissociation regions near the edges of giant molecular clouds. The total C II forbidden-line luminosity of the Galaxy is 6 x 10 to the 7th solar luminosities. It is estimated that the C II forbidden-line emitting regions consist of 4 x 10 to the 8th solar masses of hydrogen with a volume filling factor of 0.001.

Stacey, G. J.↗
NASA NTRS1986

6 CM OH absorption in megamaser galaxies

Absorption in the 2Pi sub 1/2 J = 1/2 Lambda doublet transitions of OH, 182 K above the ground state, is detected in the megamaser galaxies IC 4553 (Arp 220), MK 231, MK 273, MGC 3690, and IRAS 17208-0014. The 4660, 4751, and 4766 MHz lines have intensity ratios moderately deviating from the LTE values (1:2:1). The OH rotational temperatures appear to be close to the temperature of the dust, approx. 60 K. The common characteristics of these galaxies (absence of 6 cm inversion, the optical depths, the infrared properties, the systematic trends in the line parameters, and the rotational temperatures) all suggest that the same pump process is responsible for the 18 cm line inversion in the five megamaser sources. The inversion is probably not due to an excitation mechanism involving collisions with HI or H2. While excitation via photodissociation of H2O cannot entirely be ruled out, the most likely mechanism is considered to be to be a combination of the intense FIR field (populating higher excited OH rotational states) and the non-thermal radiation from the nuclei of the parent galaxies (affecting the excitation within the Lambda -doublets). According to an LVG model of the OH excitation of IC4553, the OH-cloud(s) have to be located close, within 200 to 300 pc, to the center of the galaxy. The excitation of the individual 18 cm lines depends critically on the effective background radiation field and hence on the galactocentric distance of the masing clump. With increasing distance first the 1720 MHz and then the 18 cm main line inversion is quenched, while 1612 MHz inversion is obtained up to approx. 600 pc. The 1612 MHz satellite line is predicted to be more intense than the 1720 MHz line. A critical test for our excitation model is to observe the 2 Pi 3/2 J = 5/2 Lambda-doublet transitions which are predicted to be detectable in absorption.

Henkel, C.↗
NASA NTRS1986

Translucent molecular clouds: Theory and observations

Few suitable stars behind molecular clouds have been identified. A limited survey was performed of interstellar lines toward highly reddened stars in the southern sky, using the ESO 1.4 m CAT telescope with a Reticon detector, and the Cerro Tololo 4 m telescope equipped with a GEC charge coupled device (CCD) detector. Because of the reduced extinction at longer wavelengths, molecules were searched for with transitions in the red part of the spectrum such as C2 and CN. For some lines-of-sight for which C2 was detected, the 4300 A line of CH was also observed. Absorption lines of interstellar C2 around 8750 A were detected in the spectra of about 1/4 of the 36 observed stars. The inferred C2 column densities range between 10 to the 13th power and 10 to the 14th power sq. cm., and are up to an order of magnitude larger than those found for diffuse clouds. The observed column densities of CH correlate very well with those of C2 over this range. In contrast, the measured column densities of CN vary by orders of magnitude between the various regions, and they do not correlate with those of C2 and CH. The observed rotational population distribution of C2 also provides information about the physical conditions in the clouds. Models of translucent molecular clouds have been constructed along the lines described by van Dishoeck and Black (1986) for diffuse clouds. The models compute accurately the fractions of atomic and molecular hydrogen as functions of depth into the clouds, as well as the excitation of H2 by ultraviolet pumping. They also incorporate a detailed treatment of the photodissociation processes of the molecules (cf. van Dishoeck 1986), which play an important role in the chemistry up to depths of about 3 mag.

Vandishoeck, E. F.↗
NASA NTRS1986

Measurement of HO2 chemical kinetics with a new detection method

Reaction rate constants of HO2+O3 were measured at various temperatures using a newly developed HO2 detection method. HO2 was detected by the OH(A-X) emission produced from photodissociative excitation of HO2 at 147 nm. In order to examine the possible interference of other emitting species with the HO2 detection, the photoexcitation processes of all the chemical species existing in the discharge flow tube were also investigated. The results are summarized.

Lee, Long C.↗