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All sourcesNASA NTRSDOE OSTI
NASA NTRS1977

Possible variations in atmospheric methane

A model coupling photochemistry and vertical transport in the troposphere has been used to investigate the magnitude of possible future perturbations to atmospheric CH4. The response of atmospheric CH4 to an increase in the concentration of CO or to a variation in stratospheric O3 is studied. Both of the above mechanisms, which could be caused by man's activities, arise because a change in the concentration of tropospheric OH will lead to a change in the CH4 abundance. The calculations imply that a perturbation of about 30-40% in atmospheric CH4 could occur if stratospheric O3 were perturbed by 10% or if man-made CO continued to increase. The possible consequences of a CH4 perturbation may entail a perturbation in stratospheric photochemistry or in the thermal balance of the atmosphere.

Chameides, W. L.↗
NASA NTRS1985

Volatiles on satellites of the outer solar system

Molecules of cosmochemically abundant elements can act as volatiles and hence play a dominant role in the climatic and surficial evolution of solid bodies. Examples on terrestrial planets are H2O on Earth and H2O and CO2 on Mars. Analogous processes in the outer solar system focussing on CH4, its associated hydrocarbons, and N2 on Titan and Triton, the large moons of Saturn and Neptune were explored. A kilometer-deep C2H6-CH4 ocean was proposed for the surface of Titan to reconcile data on the lower atmosphere with understanding of the photochemical conversion of methane to heavier hydrocarbons. If such ocean exists, then it has dissolved in it an amount of N2 equal to the present atmospheric abundance. Since N2 contributes with CH4 a substantial greenhouse effect, the atmospheric physical and chemical characteristics are strongly coupled to those of the ocean, which change with time as methane is photolyzed in the stratosphere. Some relationship exists to the runaway greenhouse model for primordial Venus and the possible climatic implications of the buffering of Earth's atmospheric CO2 by the oceans. Two important diagnostics, measurable in Titan's atmosphere, of the conditions under which icy satellites formed are the abundances of noble gases and the CHd/CH4 radio. Both of these indicators have been altered during the evolution of Titan's surface-atmosphere system, the former by interaction with the ocean and the latter by progressive photolysis of methane into heavier hydrocarbons. The physical state and composition of volatiles on the surface of Triton is controversial, but plausibly could include CH4 N2 and perhaps CO. If condensed CH4 and N2 are widespread, their transformation to and from the vapor phase dominates the surface energy balance with sunlight. The extreme seasonal modulation of subsolar latitude on Triton is thus primarily expressed by volatile transport rather than large teperature changes, with possibly drastic observational consequences. The presence of two volatile species differing greatly in their vapor pressures make Triton a crude analog of Mars. Triton might be more appropriately regarded as a deep-freeze version of Titan.

Lunine, J. I.↗
NASA NTRS1988

Measurements of argon-, helium-, hydrogen-, and nitrogen-broadened widths of methane lines near 9000 per cm

Pressure-broadened widths of rotational-vibrational lines in CH4 have been measured at very high spectral resolution in the R-branch of the 3nu3 overtone. The broadening gases were Ar, He, H2, and N2. Results are presented as averages for J-multiplets at ambient temperature. The overall values (per cm per atm) for these R-branch lines are 0.0651 (CH4-Ar), 0.0508 (CH4-He), 0.0728 (CH4-H2), and 0.0715 (CH4-N2).

Fox, Kenneth↗
NASA NTRS1989

Airborne infrared spectroscopy of Comet Wilson (1986l) and comparisons with Comet Halley

H2O and possibly CH4 have been detected in near-infrared spectra of Comet Wilson (1986l). The observed number and relative intensities of cometary H2O lines in the nu3 band at 2.65 microns were consistent with fluorescent excitation pumped by solar infrared photons. The H2O production rate in Comet Wilson was approximately 3 x 10 to the 29th/s at R = 1.2 AU; no pronounced temporal variability was observed. Lines in the nu3 band of CH4 at 3.3 microns were possibly detected at the 3 sigma confidence level. The CH4 abundance is in the range CH4/H2O = 0.014-0.045; the uncertainty is due primarily to the assumed effective excitation temperature of CH4. The CH4 abundance in this dynamically 'new' comet is similar to that observed in P/Halley. These values are low for equilibrium compositional models and very high for disequilibrium condensation in the solar nebula.

Larson, Harold P.↗
NASA NTRS1989

Spectral shifts of methane lines in collisions with hydrogen, helium, nitrogen, and argon

Pressure-induced shifts of rotational-vibrational lines in CH4 have been measured at very high spectral resolution in the R-branch of the 3nu(3) overtone. The colliding gases were H2, He, N2, and Ar. Results are presented as functions of rotational and tetrahedral quantum numbers. Mean values (in 0.001/cm per torr) for the R0-R6 multiplets are -0.01109 (CH4-H2), +0.00547 (opposite sense) (CH4-He), -0.01990 (CH4-N2), and -0.02126 (CH4-Ar).

Fox, Kenneth↗
NASA NTRS1991

Limit on the CH4/CO ratio in Comet Levy (1990c) and comparisons with other comets

Near-infrared observations of comet Levy (1900c) were made on UT 4.3 and 5.3 Sep. 1990 from the United Kingdom Infrared Telescope on Mauna Kea. A scanning Fabry-Perot interferometer in combination with a cooled grating spectrometer was used to make a sensitive search for fluorescent emission from the v zub 3 band of CH4 near lambda approx. 3.3 microns. If CH4 is a parent molecule released directly from the nucleus, then the 3 sigma limit on its abundance is CH4/H2O approx. less than 0.0031, assuming that the kinetic temperature of the inner coma is approx. 50 K and that the CH4 spin species are equilibrated at a temperature approx. greater than 50 K. Since International Ultraviolet Explorer (IUE) observations of CO in Levy indicate that CO/H2O approx. 0.04 (Feldman et al.), researchers find that CH4/CO approx. less than 0.1. Infrared spectroscopic searches for CH4 in Comet Halley also yielded no positive detections; the more sensitive upper limit from the latter observations is CH4/H2O approx. less than 0.002. Since CO/H2O approx. 0.05 in Halley (not including the extended source of CO), the upper limits on the CH4/CO ratios are almost identical for comets Levy and Halley. A marginal infrared detection of the CH4 v sub 3 band in comet Wilson yielded CH4/H2O approx. 0.01 to 0.05 (Larson et al.), but there was no positive detection of CO. If the identification of the feature in the infrared spectrum of comet Wilson is correct, then that would indicate a very high CH4/CO ratio in this comet.

Weaver, Harold A.↗
NASA NTRS1991

A sensitive upper limit on the methane abundance in Comet Levy (1990c)

Results are presented on a ground-based search for fluorescent emission from CH4 at 3.3 microns in a newly discovered long-period comet, Comet Levy (1990c). It was found that the upper limit to the CH4 abundance in Comet Levy is similar to the Comet Halley CH4 abundance estimated from lower resolution IR spectra by Kawara et al. (1988). The Comet Levy CH4 abundance is significantly lower than the abundance derived by Larson et al. (1989) from a possible detection of CH4 in Comet Wilson.

Brooke, T. Y.↗
NASA NTRS1992

Airborne flux measurements of trace species in an Arctic boundary layer

In situ airborne flux values for O3, CO, an CH4 over selected wetlands of Alaska are reported, and airborne CH4 flux measurements are presented for the first time. The source/sink distribution over the Yukon-Kuskokwim Delta (YKD) is qualitatively correlated with surface vegetation type. The CH4 source strength over the YKD ranged from 25 to 85 mg/sq m/d. A spatially averaged, seasonally adjusted source strength of 51 mg/sq m/d was established for the YKD. Indirect CH4 flux estimates obtained over the Alaskan North Slope indicate a much lower source strength. The global CH4 emission from tundra are estimated to be 44 Tg/a at an upper limit. Airborne CO flux measurements over the YKD indicate low negative flux values over the coastal areas, while some positive fluxes were observed in the inland sparsely forested regions. An inspection of the cospectrum of CO with vertical velocity for sample runs in coastal areas indicate the possibility of in situ photochemical destruction/production of CO.

Ritter, John A.↗
NASA NTRS1993

Environmental factors controlling methane emissions from peatlands in northern Minnesota

The environmental factors affecting the emission of methane from peatlands were investigated by correlating CH4 emission data for two years, obtained from five different peatland ecosystems in northern Minnesota, with peat temperature, water table position, and degree of peat humification. The relationship obtained between the CH4 flux and these factors was compared to results from a field manipulation experiment in which the water table was artificially raised in three experimental plots within the driest peatland. It was found that peat temperature, water table position, and degree of peat humification explained 91 percent of the variance in log CH4 flux, successfully predicted annual CH4 emission from individual wetlands, and predicted the change in flux due to the water table manipulation. Raising the water table in the bog corrals by an average of 6 cm in autumn 1989 and 10 cm in summer 1990 increased CH4 emission by 2.5 and 2.2 times, respectively.

Dise, Nancy B.↗
NASA NTRS1993

Upper limit on Titan's atmospheric argon abundance

An analysis is conducted on the Voyager 1 UV Spectrometer solar-occultation data and a Titan flyby spectrum of the north polar region dayglow, in order to infer the tropopausal Ar mixing ratio's upper limit as a function of the CH4 mixing ratio, f(CH4). The mole-fraction upper limit of tropopausal Ar mixing ratio ranges from 0.01 to 0.1 at f(CH4) of 0.026 to as low as 0.08 at f(CH4) of 0.05. Since the best fits to the solar occultation data require f(CH4) of more than 0.26, the Ar mixing ratio must be lower than 0.1.

Strobel, Darrell F.↗
NASA NTRS1993

Primary production control of methane emission from wetlands

Based on simultaneous measurements of CO2 and CH4 exchange in wetlands extending from subarctic peatlands to subtropical marshes, a positive correlation between CH4 emission and net ecosystem production is reported. It is suggested that net ecosystem production is a master variable integrating many factors which control CH4 emission in vegetated wetlands. It is found that about 3 percent of the daily net ecosystem production is emitted back to the atmosphere as CH4. With projected stimulation of primary production and soil microbial activity in wetlands associated with elevated atmospheric CO2 concentration, the potential for increasing CH4 emission from inundated wetlands, further enhancing the greenhouse effect, is examined.

Whiting, G. J.↗
NASA NTRS1995

Carbon isotopic analysis of atmospheric methane by isotope-ratio-monitoring gas chromatography-mass spectrometry

Less than 15 min are required for the determination of delta C(sub PDB)-13 with a precision of 0.2 ppt(1 sigma, single measurement) in 5-mL samples of air containing CH4 at natural levels (1.7 ppm). An analytical system including a sample-introduction unit incorporating a preparative gas chromatograph (GC) column for separation of CH4 from N2, O2, and Ar is described. The 15-min procedure includes time for operation of that system, high-resolution chromatographic separation of the CH4, on-line combustion and purification of the products, and isotopic calibration. Analyses of standards demonstrate that systematic errors are absent and that there is no dependence of observed values of delta on sample size. For samples containing 100 ppm or more CH4, preconcentration is not required and the analysis time is less than 5 min. The system utilizes a commercially available, high-sensitivity isotope-ratio mass spectrometer. For optimal conditions of smaple handling and combustion, performance of the system is within a factor of 2 of the shot-noise limit. The potential exists therefore for analysis of samples as small as 15 pmol CH4 with a standard deviation of less than 1 ppt.

Merritt, Dawn A.↗
NASA NTRS1996

The Surfaces of Pluto and Charon

Much of the surface of Pluto consists of high-albedo regions covered to an unknown depth by Beta-N2, contaminated with CH4, CO, and other molecules. A portion of the exposed surface appears to consist of solid H2O. The remainder is covered by lower albedo material of unknown composition. The N2 ice may occur as polar caps of large extent, leaving ices and other solids of lower volatility in the equatorial regions. The low-albedo material found primarily in the equatorial regions may consist in part of solid hydrocarbons and nitriles produced from N2 and CH4 in the atmosphere or in the surface ices. Alternatively, it may arise from deposition from impacting bodies and/or the chemistry of the impact process itself. Charon's surface is probably more compositionally uniform than that of Pluto, and is covered by H2O ice with possible contaminants or exposures of other materials that are as yet unidentified. The molecular ices discovered on Pluto and Charon have been identified from near-infrared spectra obtained with Earth-based telescopes. The quantitative interpretation of those data has been achieved through the computation of synthetic spectra using the Hapke scattering theory and the optical constants of various ices observed in the laboratory. Despite limitations imposed by the availability of laboratory data on ices in various mixtures, certain specific results have been obtained. It appears that CH4 and CO are trace constituents, and that some fraction of the CH4 (and probably the CO) on Pluto is dissolved in the matrix of solid N2. Pure CH4 probably also occurs on Pluto's surface, allowing direct access to the atmosphere. Study of the nitrogen absorption band at 2.148 micrometers shows that the temperature of the N2 in the present epoch is 40 +/-2 K. The global temperature regime of Pluto can be modeled from observations of the thermal flux at far-infrared and millimeter wavelengths. The low-albedo equatorial regions must be significantly warmer than the polar regions covered by N2 (at T = 40 K) to account for the total thermal flux measured. At the present season, the diurnal skin depth of the insolation-driven thermal wave is small, and the observed mm-wave fluxes may arise from a greater depth. Alternatively, the mm-wave flux may arise from the cool, sublimation source region. The surface microstructure in the regions covered by N2 ice is likely governed by the sintering properties of this highly volatile material. The observed nitrogen infrared band strength requires that expanses of the surface be covered with cm-sized crystals of N2. Grains of H2O ice on Charon, in contrast, are probably of order 50 micrometers in size, and do not metamorphose into larger grains at a significant rate. Because of the similarities in size, density, atmosphere and surface composition between Pluto and Neptune's satellite Triton, the surface structures observed by Voyager on Triton serve as a plausible paradigm for what might be expected on Pluto. Such crater forms, tectonic structures, aeolian features, cryovolcanic structures, and sublimation-degraded topography as are eventually observed on Pluto and Charon by spacecraft will give information on their interior compositions and structures, as well as on the temperature and wind regimes over the planet's extreme seasonal cycle.

Cruikshank, Dale P.↗
NASA NTRS1995

The Surface Compositions of Triton, Pluto, and Charon

Neptune's satellite Triton, and the planet-satellite binary Pluto and Charon, are the most distant planetary bodies on which ices have been directly detected. Triton and Pluto have very similar dimensions and mean densities, suggesting a similar or common origin. Through earth-based spectroscopic observations in the near-infrared, solid N2, CH4, and CO have been found on both bodies, with the additional molecule C02 on Triton. N2 dominates both surfaces, although the coverage is not spatially uniform. On Triton, the CH4 and CO are mostly or entirely frozen in the N2 matrix, while CO2 may be spatially segregated. On Pluto, some CH4 and the CO are frozen in the N2 matrix, but there is evidence for additional CH4 in a pure state, perhaps lying as a lag deposit on a subsurface layer of N2. Despite their compositional and dimensional similarities, Pluto and Triton are quite different from one another in detail. Additional hydrocarbons and other volatile ices have been sought spectroscopically but not yet have been detected. The only molecule identified on Pluto's satellite Charon is solid H2O, but the spectroscopic data are of low precision and admit the presence of other ices such as CH4.

Cruikshank, Dale P.↗
NASA NTRS2002

Synthesis of HCN and HNC in Ion-Irradiated N2-Rich Ices

Near-IR observations reveal that N2-rich ice containing small amounts of CH4, and CO, is abundant on the surfaces of Triton, a moon of Neptune, and Pluto. N2-rich ices may also exist, in interstellar environments. To investigate the radiation chemistry of such ices we performed a systematic IR study of ion-irradiated Nz-rich mixtures containing CH4 and CO. Irradiation of N2 + CH4 mixtures at 12 K, showed that HCN, HNC, diazomethane, and NH3 were produced. We also found that UV photolysis of these ices produced detectable HCN and HNC. Intrinsic band strengths, A(HCN) and A(HNC), were measured and used to calculate yields of HCN and HNC. Similar results were obtained on irradiation of N2 + CH4 + CO ices at 12 K, with the main difference being the formation of HNCO. In all cases we observed changes on warming. For example, when the temperature of irradiated Nz + CH4 + CO was raised from 12 to 30 K, HCN, HNC, and HNCO reacted with NH3, and OCN-, CN-, N3-, and NH4+ were produced. These ions, appearing at 30 K, are expected to form and survive on the surfaces of Triton, Pluto, and interstellar grains. Our results have astrobiological implications since some of these radiation products are involved in the syntheses of biomolecules such as amino acids and peptides.

Moore, M. H.↗
NASA NTRS2003

Physical Studies of Brown Dwarfs and Extrasolar Planets

The primary activities supported under this grant included research into the mid-infrared spectral properties of brown dwarfs, with particular emphasis on the 3-4 micron region, the L band. Several observing trips were made to use facilities on Mauna Kea. The primary discovery was the detection of absorption due to CH4 in several L dwarfs, including one classified as an L5. This is significant since CH4 is usually considered to be the defining characteristic of T dwarfs. The stronger fundamental band at 3.3um, however, makes it possible to observe the emergence of CH4 at hotter temperatures. A secondary result of this work is the surprising weakness of the CH4 nu3 band. This can be interpreted as either an indication that derived effective temperatures are too low, or perhaps, that the equilibrium abundance of CH4 is suppressed due to non-equilibrium processes at work in the atmosphere.

Boyce, Joseph↗
NASA NTRS1997

A blast of gas in the latest Paleocene: simulating first-order effects of massive dissociation of oceanic methane hydrate

Carbonate and organic matter deposited during the latest Paleocene thermal maximum is characterized by a remarkable -2.5% excursion in delta 13C that occurred over approximately 10(4) yr and returned to near initial values in an exponential pattern over approximately 2 x 10(5) yr. It has been hypothesized that this excursion signifies transfer of 1.4 to 2.8 x 10(18) g of CH4 from oceanic hydrates to the combined ocean-atmosphere inorganic carbon reservoir. A scenario with 1.12 x 10(18) g of CH4 is numerically simulated here within the framework of the present-day global carbon cycle to test the plausibility of the hypothesis. We find that (1) the delta 13C of the deep ocean, shallow ocean, and atmosphere decreases by -2.3% over 10(4) yr and returns to initial values in an exponential pattern over approximately 2 x 10(5) yr; (2) the depth of the lysocline shoals by up to 400 m over 10(4) yr, and this rise is most pronounced in one ocean region; and (3) global surface temperature increases by approximately 2 degrees C over 10(4) yr and returns to initial values over approximately 2 x 10(6) yr. The first effect is quantitatively consistent with the geologic record; the latter two effects are qualitatively consistent with observations. Thus, significant CH4 release from oceanic hydrates is a plausible explanation for observed carbon cycle perturbations during the thermal maximum. This conclusion is of broad interest because the flux of CH4 invoked during the maximum is of similar magnitude to that released to the atmosphere from present-day anthropogenic CH4 sources.

Non-NASA Center↗
NASA NTRS2005

Near Infrared Spectra of Mixtures Relevant to Icy Satellites

We will present near IR spectra of ice mixtures and review the differences between spectra of mixtures and those of pure solids: the creation of new features, weakening and shifting of bands, dependence on concentration, and changes with temperature. The forbidden CO2 (2nu3) overtone at 2.134 microns (4685/cm) is absent from the spectrum of pure CO2, but present in all of the following mixtures: H2O/CO2 = 5 and = 25, H2O:CH3OH:CO2 = 100:2.5:1, and CH3OH:CO2 = 5. Also, in mixtures of H2O and any other material, we see a feature at 1.89 microns (5290/cm) that is possibly related to the "dangling OH" feature at 2.73 microns (3360/cm). The features of a material in H2O are generally weaker and shifted to longer wavelength in comparison to the pure substance. For example, the largest near-IR absorption of pure solid CH4 is located at 2.324 microns (4303/cm) but is broader and at slightly longer wavelength in samples mixed with H2O. The degree of shifting and weakening depends on the ratio of the mixture. The mixture mentioned above was at a ratio of H2O/ CH4 = 3. When the ratio rises to H2O/ CH4 = 87, the CH4 feature at 2.324 microns is shifted to shorter wavelength and is much broader and weaker. In CH4/ H2O mixtures the peaks shift to higher frequency and become increasingly broad, but this trend is reversible on re-cooling, even though the phase transitions of H2O are irreversible. In short, mixtures created in the lab produce spectra that are very different from modeled combinations of end member species. Recent Cassini VIMS observations show the CO2 fundamental at 4.255 microns (2350/cm) on Iapetus [l] and at 4.26 microns (2347/cm) on Phoebe [2], while Galileo NIMS observed it at 4.25 microns (2353/cm) on Ganymede [3]. Since pure CO2 is located at 4.266 (2344/cm), the CO2 must be mixed with something else to produce the shift. A mixture of CH3OH:CO2 = 5 at 90 K shifts the fundamental to 4.262 microns (2346/cm). The shifts in the feature between satellites could indicate variations in concentration and temperature, or the introduction of a new compound, encouraging further lab investigation.

Mastrapa, Rachel M. E.↗