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A fast-response instrument for monitoring CH4 was designed and tested using a modified nondispersive infrared technique. An analysis of the single-beam rotating-cell system is presented along with the signal processing circuit. A calibration of the instrument shows that the technique can be used to measure CH4 concentrations as small as 5 ppm-m and the effects of interfering gases are analyzed.
Value and limitations of transition-state theory (TST) are reviewed. TST analyses of the temperature dependence of the 'direct' reactions CH3 + CH3CHO yields CH4 + CH3CO(1) and O + CH4 yields OH + CH3(2) are presented in detail, and other examples of TST usefulness are recalled. Limitations are discussed for bimolecular processes in terms of 'complex' vs. 'direct' mechanisms. The reaction OH + CO yields CO2 + H is discussed in this context. Limitations for unimolecular processes seem to arise only for simple bond fission processes, and recent advances are noted.
New narrow-band (100 A) photoelectric slit scan photometry of Uranus has been obtained in the spectral region 6000 to 8500 A. Coarse radial intensity profiles in seven wavebands are presented. Results of the investigation confirm earlier studies of limb brightening on the Uranus disk, but not all strong CH4 absorption bands are found to exhibit limb brightening. Specifically, the CH4 bands at 8000 and 8500 A show pronounced apparent limb darkening. Polar brightening may be responsible for the phenomenon. If so, an aerosol haze with a local optical thickness of approximately 0.5 or greater would be required. Visibility of the dense cloud layer located deep in the atmosphere might also cause apparent limb darkening. If so, the maximum permitted CH4/H2 mixing ratio in the visible atmosphere would correspond to 3 times the solar value.
The spectrum of sunlight reflected by Jupiter is analyzed by comparing observations of Woodman (1979) with multiple-scattering computations. The analysis yields information on the vertical cloud structure at several latitudes and on the abundance of CH4 and NH3 in the atmosphere of Jupiter. The abundances of CH4 and NH3 suggest that all ices and rocks are overabundant on Jupiter by a factor of 2 or more, providing an important constraint on models for the formation of Jupiter from the primitive solar nebula. The pressure level of the clouds, the gaseous NH3 abundance, the mean temperature profile, and the Clausius-Clapeyron relation suggest that these clouds are predominantly ammonia crystals with the cloud bottom at 600-700 mb. A diffuse distribution of aerosols exists between 150 and 500 mb, and the spectral variation of albedo reflects a changing bulk absorption coefficient of the material composing the aerosols and is diagnostic of the aerosol composition.
A laboratory gas analysis system was developed specifically to make trace level measurements of carbon monoxide. To assure that the data collected with this system are correctly aligned with other established methods for making these measurements, an intercalibration study was conducted. The calibration gas was analyzed by the various participating laboratories and found to contain 1.28 ppm CO. Samples were collected at 25 deg, 35 deg, and 45 deg N for profile data to study the variation in concentrations of CO and CH4 as a function of altitude and latitude in continental air over the eastern seaboard of the United States. The experiment was repeated several months later to determine if there were seasonally dependent variations in the CO and CH4 concentrations.
A new atlas of CH4 lines in the 1120-1800-per cm region has been generated, based on laboratory spectra taken with a Nicolet interferometer at 0.06-per cm resolution with 635-cm path length at pressures of 0.98 torr, 4.86 torr, and 19.97 torr. A compilation of line positions and line intensities includes 1339 CH4 lines, several hundred of which have not been previously observed.
A low-resolution infrared spectrum of Triton in the region 1.4-2.6 microns shows a broad absorption at 2.3 microns which is attributed to gaseous methane. The computed surface partial pressure of CH4, based on a random band model extrapolation of new laboratory spectra, is (1 + or - 0.5) times 10 to the -4th bars, a value consistent with the calculated vapor pressure of methane gas above methane ice at the expected temperature of Triton. There is, however, no compelling evidence for the presence of solid CH4 on the satellite's surface.
Saturn's 3nu3 CH4 band has been reobserved during April-June 1976, using the same telescope and spectrographic set-up used to study this band during the 1970 apparition. Direct comparison of the ratio spectra Saturn/moon reveals greater absorption in the manifold cores during 1976, but the increase is not as pronounced as that for the stronger CH4 bands. The rotational temperature and effective pressure of this band did not change significantly. These results are interpreted in terms of a possibly seasonal settling of the upper boundary of Saturn's atmospheric haze layer.
Features taken from various models of Titan's atmosphere are combined in a working composite model that provides environmental constraints within which different pathways for organic chemical synthesis are determined. Experimental results and theoretical modeling suggest that the organic chemistry of the satellite is dominated by two processes: photochemistry and energetic particle bombardment. Photochemical reactions of CH4 in the upper atmosphere can account for the presence of C2 hydrocarbons. Reactions initiated at various levels of the atmosphere by cosmic rays, Saturn 'wind', and solar wind particle bombardment of a CH4-N2 atmospheric mixture can account for the UV-visible absorbing stratospheric haze, the reddish appearance of the satellite, and some of the C2 hydrocarbons. In the lower atmosphere photochemical processes will be important if surface temperatures are sufficiently high for gaseous NH3 to exist. It is concluded that the surface of Titan may contain ancient or recent organic matter (or both) produced in the atmosphere.
Observations of Uranus during the 1975, 1976, and 1978 apparitions reveal a weak absorption at the wavelength of the R5(1) line of HD with equivalent width 1.0 + or - 0.4 mA. The D/H ratio in Uranus' atmosphere implied by this line and other published spectra is (0.000048 + or - 0.000015), and may not be significantly different from that in the atmospheres of Jupiter and Saturn. In addition, the spectra exhibit two weak absorptions at 6044.76 + or - 0.02 and 6045.54 + or 0.02 A which were not identifiable. No trace of absorption is visible near these wavelengths or near the HD wavelength in a laboratory spectrum of 4.92 km-am CH4 which was obtained in an attempt to identify these absorption features and to verify that the HD feature does not arise from CH4.
Laboratory band-model absorption coefficients of CH4 were used to calculate the Uranus spectrum from 5400 to 10,400 A. A good fit for both strong and weak bands for the Uranus spectrum over the entire wavelength interval was achieved; three atmospheric models were employed: (1) a reflecting layer model; (2) a homogeneous scattering layer model; and (3) a clear atmosphere sandwiched between two scattering layers. The spectrum for the reflecting layer model shows serious discrepancies but indicates that large amounts of CH4 are necessary to reproduce the Uranus spectrum. Both scattering models gave reasonably good fits; the homogeneous model requires a particle scattering albedo of at least 0.998 and an abundance per scattering mean free path of about 1 km-am. For the sandwich model, a continuum single scattering albedo of 0.995 was derived for the upper scattering layer, and the scattering optical depth variable wavelength was consistent with Rayleigh scattering.
Anaerobic and aerobic sporeformers and non-sporeformers were cultivated anaerobically in nutrient media under various pressures (up to 1800 psi) of pure H2, CH4, NH3, and H2S. Viability assays were performed periodically to determine growth, survival, or spore survival. Hydrogen up to 1800 psi demonstrated little or no suppression of growth with the possible exception of Bacillus coagulans at 1800 psi. The obligate anaerobes grew very well. Under CH4 the obligate anaerobes again exhibited the most prolific growth, whereas the facultative anaerobes grew well except under higher pressures. Ammonia at low pressure was extremely toxic to all test organisms. At 100 psi all populations were killed within 24 hours except Staphylococcus aureus which survived for 72 hours and the Bacillus spp. which produced a surviving population of approximately 10,000 spores/ml. All populations in H2S were killed within 24 to 48 hours except Proteus mirabilis which decreased to 100 cells/ml and the Bacillus spp. Spore survival studies of two months duration demonstrated that B. coagulans and B. pumilus survived under all experimental conditions. Clostridium novyi type B and C. sporogenes were killed rapidly in NH3 and H2S and demonstrated no sporulation.
The possible synthesis of organic molecules by the absorption of galactic cosmic rays in an N2-CH4-H2 Titan model atmosphere has been studied. The cosmic-ray-induced ionization results in peak electron densities of 2000/cu cm, with NH(+), C3H9(+), and C4H9(+) being among the important positive ions. Details of the ion and neutral chemistry relevant to the production of organic molecules are discussed. The potential importance of N(2D) reactions with CH4 and H2 is also demonstrated. Although the integrated production rate of organic matter due to the absorption of the cosmic ray cascade is much less than that by solar ultraviolet radiation, the production of nitrogen-bearing organic molecules by cosmic rays may be greater.
Processes that affect the concentration of tropospheric OH are considered, taking into account linkages between the chemistry of OH and the chemistry of H, HO2, and H2O2. A review is presented of observational data of special relevance to OH, notably the distributions of CO, CH4, O3, H2O, HNO3, NO, and NO2. Most of the results presented in connection with the description of the model were obtained by solving time-dependent continuity equations. Rates for photolytic processes were allowed to vary diurnally with insolation. It is found that a well-calibrated and reliable model for OH places important constraints on global budgets for a variety of gases including CH4, H2, and CH3Cl in addition to CO. Accurate measurements of species such as CH3CCl3 can provide valuable checks on global models that must integrate over a variety of atmospheric conditions. However, emission rates for the relevant gases must be adequately quantified.
Jupiter's reflectivity was measured as a function of wavelength between 3000 and 10,500 Angstrom for two nights during the 1979 apparition. The spectra obtained were used to calibrate the wavelength response of Voyager images and to establish differences from previous apparitions. The observations were taken in the prominent belts and zones and both polar caps along the central meridian using a slit of dimensions 2.33 x 2.5 sq arcsec. The equivalent widths of the 6190 and 7270 Angstrom CH4 bands were measured; compared to the 1976 apparition, there was significantly less CH4 absorption in the north tropical zone. Such equivalent-width decreases are said to result from either a reduction in particle albedo or a decrease in the scattering mean free path owing to a greater concentration of aerosol particles in the NTrZ.
Plots of absorption line strength versus line position for wavenumbers from 0 to 17,900 cm(-1) are shown for 20 atmospheric gases (H2O, CO2, O3, N2O, CO, CH4, O2, NO, SO2, NO2, NH3, HNO3, OH, HF, HCl, HBr, HI, ClO, OCS, H2CO). Also shown are similar plots of lower-state energy values for adsorption lines for the strongly adsorbing atmospheric gases (H2O, CO2, O3, and CH4) for wavenumbers from 0 to 5000 cm(-1).
Near-infrared spectrophotometry of Triton and Pluto at low spectral resolution and signal precision reveals methane absorption on both bodies. The absorption on Triton is probably gaseous CH4, while that on Pluto is a combination of gas and ice of CH4. Using present detectors and telescopes, spectra of Triton and Pluto can be obtained which are 5-10 times better than those published, but such data will not be sufficient to distinguish between gaseous and solid methane on these bodies.
Activation energies are calculated by the bond-energy-bond-order (BEBO) and the bond-strength-bond-length (BSBL) methods for the reactions of C2H radicals with H2, CH4, and C2H6 and for the reactions of CN radicals with H2 and CH4. The BSBL technique accurately predicts the activation energies for these reactions while the BEBO method yields energies averaging 9 kcal higher than those observed. A possible reason for the disagreement is considered.