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1.
Close to 2000 laboratory measurements of the microwave opacity and refractivity of gaseous NH3 in an H2/He atmosphere have been conducted in the 1.1-20 cm wavelength range (1.5-27 GHz) at pressures from 30 mbar to 12 bar and at temperatures from 184 to 450 K. The mole fraction of NH3 ranged from 0.06 to 6% with some additional measurements of pure NH3. The high accuracy of these results have enabled development of a new model for the opacity of NH3 in a H2/He atmosphere under jovian conditions. The model employs the Ben-Reuven lineshape applied to the published inversion line center frequencies and intensities of NH3 (JPL Catalog—[Pickett, H.M., Poynter, R.L., Cohen, E.A., Delitsky, M.L., Pearson, J.C., Müller, H.S.P., 1998. J. Quant. Spectrosc. Radiat. Trans. 60, 883-890]) with empirically-fitted line parameters for H2 and He broadening, and for the self-broadening of some previously unmeasured ammonia inversion lines. The new model for ammonia opacity will provide reliable results for temperatures from 150 to 500 K, at pressures up to 50 bar and at frequencies up to 40 GHz. These results directly impact the retrieval of jovian atmospheric constituent abundances from the Galileo Probe radio signal absorption measurements, from microwave emission measurements conducted with Earth-based radio telescopes and with the future NASA Juno mission, and studies of Saturn's atmosphere conducted with the Cassini Radio Science Experiment and the Cassini RADAR 2.1 cm passive radiometer. 相似文献
2.
We report measurements of the Jupiter brightness spectrum in the 850-μm and 1100-μm atmospheric windows with a spectral resolution of 125 MHz, obtained with a Fourier transform spectrometer on the James Clerk Maxwell Telescope. Three results were obtained. First, the predicted absorption features due to the rotational lines of HCN at 266 and 354 GHz were not detected within our error limits of less than 1%. We establish new upper limits for the HCN abundance in the jovian troposphere for five assumed abundance distributions and for two assumed NH3abundances. The upper limits are 1.7 to 13 times smaller than the abundance value obtained in the only reported detection of HCN in Jupiter prior to the impact of Shoemaker–Levy 9. Second, the continuum brightness temperature spectrum at 850 μm was determined and is in agreement with previous measurements, but has large error bars due to uncertainties in the photometric calibration. We estimate the ammonia abundance in the 1–2 bar region to be 1.7 times solar, but this result is tentative since scattering by NH3cloud particles and absorption by gaseous H2S were neglected in our atmospheric model. Finally, the first rotational line of PH3at 267 GHz was not detected, a result which we demonstrate is consistent with the statistical noise level in these measurements, with current values of the spectroscopic parameters, and with phosphine measurements at other wavelengths. 相似文献
3.
Detection and measurement of atmospheric water vapor in the deep jovian atmosphere using microwave radiometry has been discussed extensively by Janssen et al. (Janssen, M.A., Hofstadter, M.D., Gulkis, S., Ingersoll, A.P., Allison, M., Bolton, S.J., Levin, S.M., Kamp, L.W. [2005]. Icarus 173 (2), 447-453.) and de Pater et al. (de Pater, I., Deboer, D., Marley, M., Freedman, R., Young, R. [2005]. Icarus 173 (2), 425-447). The NASA Juno mission will include a six-channel microwave radiometer system (MWR) operating in the 1.3-50 cm wavelength range in order to retrieve water vapor abundances from the microwave signature of Jupiter (see, e.g., Matousek, S. [2005]. The Juno new frontiers mission. Tech. Rep. IAC-05-A3.2.A.04, California Institute of Technology). In order to accurately interpret data from such observations, nearly 2000 laboratory measurements of the microwave opacity of H2O vapor in a H2/He atmosphere have been conducted in the 5-21 cm wavelength range (1.4-6 GHz) at pressures from 30 mbars to 101 bars and at temperatures from 330 to 525 K. The mole fraction of H2O (at maximum pressure) ranged from 0.19% to 3.6% with some additional measurements of pure H2O. These results have enabled development of the first model for the opacity of gaseous H2O in a H2/He atmosphere under jovian conditions developed from actual laboratory data. The new model is based on a terrestrial model of Rosenkranz et al. (Rosenkranz, P.W. [1998]. Radio Science 33, 919-928), with substantial modifications to reflect the effects of jovian conditions. The new model for water vapor opacity dramatically outperforms previous models and will provide reliable results for temperatures from 300 to 525 K, at pressures up to 100 bars and at frequencies up to 6 GHz. These results will significantly reduce the uncertainties in the retrieval of jovian atmospheric water vapor abundances from the microwave radiometric measurements from the upcoming NASA Juno mission, as well as provide a clearer understanding of the role deep atmospheric water vapor may play in the decimeter-wavelength spectrum of Saturn. 相似文献
4.
Sulfur dioxide has a strong and complex rotational spectrum in the microwave and far infrared regions. The microwave absorption due to SO2 in a CO2 mixture is calculated for conditions applicable to the Venus atmosphere. It is shown that at the concentrations detected by Pioneer-Venus in situ measurements, SO2 may be expected to contribute significantly to the microwave opacity of the Venus atmosphere. In particular, SO2 might provide the major source of opacity in the atmospheric region immediately below the main sulfuric acid cloud deck. The spectrum is largely nonresonant at the pressures where SO2 is expected to occur, however. 相似文献
5.
Photolysis of NH3PH3 mixtures (11 Torr) at 175°K resulted in the same initial rate of P2H4 formation as when the 11 Torr of pure PH3 was photolyzed. A higher yield of P2H4 is obtained at 175°K than at 298°K because some of the P2H4 condenses on the cell wall at 175°K and is not subject to further reaction. Some reaction of P2H4 is taking place as observed by the decrease in its yield and on the formation of red phosphorus on extended photolysis of PH3 at 175°K. No NH2PH2 or (PN)x were detected as photoproducts as indicated by the absence of change in the UV spectral properties of the P2H4 and red phosphorus fraction, respectively, when NH3 is present. Although the pathway for PH3 decomposition is changed, the outcome of the photochemical process is essentially the same in the absence or presence of NH3. The formation of P2H4 and red phosphorus was not inhibited by small amounts of C2H4 and C2H2, so the low levels of hydrocarbons on Jupiter and Saturn will not have a significant effect on the course of PH3 photolysis. The ratio of products of PH3 photolysis are only slightly affected by the wavelength of light used. Use of xenon lamp, with a continuous emission in the ultraviolet where P2H4 absorbs, results in only a modest decrease in the yield of P2H4 and a modest increase in the rate of formation of red phosphorus as compared to the rates observed with a 206.2-nm light source. The quantum yield for P2H4 formation is pressure independent in the 0.5–11 Torr range. This quantum yield is not affected by lowering the temperature to 157°K or by the addition of 100 Torr of H2. It is concluded that photolysis of PH3 to P2H4 and the subsequent conversion of P2H4 to red phosphorus are likely procses on Jupiter and Saturn and that particles of P2H4 condense in the atmospheres of these planets. The conversion of some of the P2H4 to red phosphorus may take place on Jupiter. 相似文献
6.
Since the original suggestion by Gillett et al. (1969) it has generally been assumed that the region of partial transparency near 5 μm in Jupiter's atmosphere (the 5-μm window) is bounded by the v4 NH3 at 6.1 μm and the v3 CH4 band at 3.3 μm. New measurements of Jupiter and of laboratory phosphine (PH3) samples show that PH3 is a significant contributor to the continuum opacity in the window and in fact defines its short-wavelength limit. This has important implications for the use of 5-mu;m observations as a means to probe the deep atmospheric structure of Jupiter. The abundance of PH3 which results from a comparison of Jovian and laboratory spectra is about 3 to 5 cm-am. This is five to eight times less than that found by Larson et al. [Astrophys. J. (1977) 211, 972–979] in the same spectral region, but is in good agreement with the result of Tokunaga et al. [Astrophys. J. (1979) 232, 603–615] from 10-μm observations. 相似文献
7.
The flux emitted by Titan's disk in millimeter lines of HCN, HC3N, CH3CN, and CO is calculated by means of a radiative transfer formulation which takes into account the sphericity of the atmosphere. It is demonstrated that the plane-parallel approximation for radiative transfer is no longer valid, especially in the core of emission lines, when Titan is not spatially resolved. The antenna temperatures which would be measured by large radiotelescopes observing Titan at frequencies of (1?0) and (2?1) transitions of CO, of (1?0), (2?1), and (3?2) transitions of HCN, and of selected transitions of HC3N and CH3CN in the range 80–300 GHz are calculated. The observability of these transitions is investigated. It is concluded that there is the possibility of inferring the vertical stratospheric distribution of these species from line shape measurements to be achieved with existing or forthcoming radioastronomical instrumentation. The determination of the CO abundance by D. O. Muhleman, G. L. Berge, and R. T. Clancy (1984, (Science (Washington, D.C.), 223, 393–396) from measurements at 115.3 GHz in two 200 MHz bands, is reinterpreted by means of this radiative transfer formulation. A CO mixing ratio between 3 × 10?5 and 18 × 10?5, with a most plausible value of 7.5 × 10?5, is found. 相似文献
8.
Over 1000 laboratory measurements of the 2-4 mm-wavelength opacity of ammonia have been made under simulated jovian atmospheric conditions using a high-precision laboratory system developed at Georgia Tech. These laboratory measurements of the opacity of ammonia were made of various gas mixtures of hydrogen (∼77.5-85.5%), helium (∼12.5-13.5%), and ammonia (1-10%) at pressures between 1 and 3 bars and temperatures between 200 and 300 K. Laboratory measurements were also made of the opacity of pure ammonia at pressures between 0.05 and 1 bar and temperatures between 200 and 300 K. Using these millimeter-wavelength measurements and close to 2000 cm-wavelength measurements made by Hanley et al. (2009), a new consistent model has been developed to accurately characterize the absorption spectra of ammonia in a hydrogen/helium atmosphere in the 1 mm to 30 cm wavelength range. This model can be used in the 1-30 cm wavelength range at pressures up to 20 bars and temperatures from 200 to 500 K and in the 1 mm to 1 cm wavelength range at pressures up to 3 bars and temperatures from 200 to 300 K. These measurements and the accompanying model will enable better interpretation of the centimeter- and millimeter-wavelength emission spectra of the jovian planets. 相似文献
9.
We have used synthetic spectra to analyze a medium resolution 2.9-4.2 μm spectrum of Saturn's temperate region observed at UKIRT using CGS4. The synthetic spectra include CH4, PH3, and NH3 lines, for which mixing ratios were adopted from recent Cassini results. The observed absorption features in the spectrum are well accounted for by lines of these molecular species formed 22 +/− 8 km above the 1 bar pressure level at ∼610 mbar. The influence of optically thin haze particles at higher altitudes on the spectrum is not pronounced, with higher spectral resolution probably required to constrain the effects of haze in this wavelength region. Fluorescent line emission by CH4 in its ν3 and ν3+ν4−ν4 bands, detected in the 3.2-3.5 μm region, originates between 400 km (∼0.06 mbar) and 800 km (∼0.01 μbar) above the 1 bar level, with peak contributions from the two major contributing bands at 550 km (∼3 μbar) and 700 km (∼0.1 μbar), respectively. 相似文献
10.
The abundances of PH3, CH3D, and GeH4 are derived from the 2100- to 2250-cm?1 region of the Voyager 1 IRIS spectra. No evidence is seen for large-scale variations of the phosphine abundance over Jovian latitudes between ?30 and +30°. In the atmospheric regions corresponding to 170–200°K, the derived PH3/H2 value is (4.5 ± 1.5) × 10?7 or 0.75 ± 0.25 times the solar value. This result, compared with other PH3 determinations at 10 μm, suggests than the PH3/H2 ratio on Jupiter decreases with atmospheric pressure. In the 200–250°K region, we derive, within a factor of 2, CH3D/H2 and GeH4/H2 ratios of 2.0 × 10?7 and 1.0 × 10?9, respectively. Assuming a C/H value of 1.0 × 10?3, as derived from Voyager, our CH3D/H2 ratio implies a D/H ratio of 1.8 × 10?5, in reasonable agreement with the interstellar medium value. 相似文献
11.
Leigh N. Fletcher Kevin H. Baines Adam P. Showman Glenn S. Orton C. Merlet 《Icarus》2011,214(2):510-533
The latitudinal variation of Saturn’s tropospheric composition (NH3, PH3 and AsH3) and aerosol properties (cloud altitudes and opacities) are derived from Cassini/VIMS 4.6-5.1 μm thermal emission spectroscopy on the planet’s nightside (April 22, 2006). The gaseous and aerosol distributions are used to trace atmospheric circulation and chemistry within and below Saturn’s cloud decks (in the 1- to 4-bar region). Extensive testing of VIMS spectral models is used to assess and minimise the effects of degeneracies between retrieved variables and sensitivity to the choice of aerosol properties. Best fits indicate cloud opacity in two regimes: (a) a compact cloud deck centred in the 2.5-2.8 bar region, symmetric between the northern and southern hemispheres, with small-scale opacity variations responsible for numerous narrow light/dark axisymmetric lanes; and (b) a hemispherically asymmetric population of aerosols at pressures less than 1.4 bar (whose exact altitude and vertical structure is not constrained by nightside spectra) which is 1.5-2.0× more opaque in the summer hemisphere than in the north and shows an equatorial maximum between ±10° (planetocentric).Saturn’s NH3 spatial variability shows significant enhancement by vertical advection within ±5° of the equator and in axisymmetric bands at 23-25°S and 42-47°N. The latter is consistent with extratropical upwelling in a dark band on the poleward side of the prograde jet at 41°N (planetocentric). PH3 dominates the morphology of the VIMS spectrum, and high-altitude PH3 at p < 1.3 bar has an equatorial maximum and a mid-latitude asymmetry (elevated in the summer hemisphere), whereas deep PH3 is latitudinally-uniform with off-equatorial maxima near ±10°. The spatial distribution of AsH3 shows similar off-equatorial maxima at ±7° with a global abundance of 2-3 ppb. VIMS appears to be sensitive to both (i) an upper tropospheric circulation (sensed by NH3 and upper-tropospheric PH3 and hazes) and (ii) a lower tropospheric circulation (sensed by deep PH3, AsH3 and the lower cloud deck). 相似文献
12.
The Sardinia Radio Telescope (SRT) is a challeging scientific project managed by the National Institute for Astrophysics (INAF),
it is being developed at 30 km North of the city of Cagliari, Italy. The goal of the SRT project is to build a general purpose,
fully steerable, 64 m diameter radio telescope, capable of operating with high efficiency in the centimeter and millimeter
frequency range (0.3–100 GHz). In portions of this frequency range, especially towards the high end, astronomical observations
can be heavily deteriorated by non-optimal atmospheric conditions, especially by water vapor content. The water molecule permanent
electric dipole in fact, leads to pressure broadened rotational transitions around the 22.23 GHz spectral line. Furthermore,
water vapor’s continuum absorption and emission may influence higher frequency observations too. To a lower degree, cloud
liquid black body radiation can also affect centimeter and millimeter observations. In addition to this, inhomogeneities in
water vapor distributions can cause signal phase errors which introduce a great amount of uncertainty to VLBI mode observations.
The Astronomical Observatory of Cagliari (OA-CA) has obtained historical timeseries of radiosonde profiles conducted at the
airport of Cagliari. Through the radiosonde measurements and an appropriate radiative transfer model, we have performed a
statistical analysis of the SRT site’s atmosphere which accounts for atmospheric opacity at different frequencies, integrated
water vapor (IWV), integrated liquid water (ILW) and cloud cover distributions during the year. This will help to investigate
in which period of the year astronomical observations at different frequencies should be performed preferably. The results
show that, at the SRT site, K-band astronomical observations are possible all year round, the median opacity at 22.23 GHz
is 0.10 Np in the winter (Dec-Jan-Feb) and 0.16 Np in the summer (Jun-Jul-Aug). Integrated water vapor during winter months
ranges, on average, between 7 and 15 mm. Cloud cover is usually not present for more than 36% of the time during the year.
The atmospheric opacity study indicates that observations at higher frequencies (50–100 GHz) may be performed usefully: the
median opacity at 100 GHz is usually below or equal to 0.2 Np in the period that ranges from January to April. 相似文献
13.
We report observation and analysis of a high-resolution 2.87-3.54 μm spectrum of the southern temperate region of Saturn obtained with NIRSPEC at Keck II. The spectrum reveals absorption and emission lines of five molecular species as well as spectral features of haze particles. The ν2+ν3 band of CH3D is detected in absorption between 2.87 and 2.92 μm; and we derived from it a mixing ratio approximately consistent with the Infrared Space Observatory result. The ν3 band of C2H2 also is detected in absorption between 2.95 and 3.05 μm; analysis indicates a sudden drop in the C2H2 mixing ratio at 15 mbar (130 km above the 1 bar level), probably due to condensation in the low stratosphere. The presence of the ν3+ν9+ν11 band of C2H6 near 3.07 μm, first reported by Bjoraker et al. [Bjoraker, G.L., Larson, H.P., Fink, U., 1981. Astrophys. J. 248, 856-862], is confirmed, and a C2H6 condensation altitude of 10 mbar (140 km) in the low stratosphere is determined. We assign weak emission lines within the 3.3 μm band of CH4 to the ν7 band of C2H6, and derive a mixing ratio of 9±4×10−6 for this species. Most of the C2H6 3.3 μm line emission arises in the altitude range 460-620 km (at ∼μbar pressure levels), much higher than the 160-370 km range where the 12 μm thermal molecular line emission of this species arises. At 2.87-2.90 μm the major absorber is tropospheric PH3. The cloud level determined here and at 3.22-3.54 is 390-460 mbar (∼30 km), somewhat higher than found by Kim and Geballe [Kim, S.J., Geballe, T.R., 2005. Icarus 179, 449-458] from analysis of a low resolution spectrum. A broad absorption feature at 2.96 μm, which might be due to NH3 ice particles in saturnian clouds, is also present. The effect of a haze layer at about 125 km (∼12 mbar level) on the 3.20-3.54 μm spectrum, which was not apparent in the low resolution spectrum, is clearly evident in the high resolution data, and the spectral properties of the haze particles suggest that they are composed of hydrocarbons. 相似文献
14.
A spectrum of Jupiter between 6000 and 12 000 cm? at high resolution (0.05 cm?) was recorded with a Michelson interferometer at Palomar Mountain in October 1974. An analysis of the R branch of the 3ν3CH4 band with the reflecting-layer model, taking into account the H2 absorption which occurs in the same spectral range, leads to a Lorentzian half-width of 0.09 ± 0.02 cm?1, a rotational temperature of 175 ± 10° K, and a CH4 abundance of order 52m atm. Five lines of the 13CH43ν3 band have been identified; a comparison with new laboratory spectra indicates that the 13CH4/12CH4 ratio in the Jupiter atmosphere is close to the terrestrial ratio. 相似文献
15.
The global distribution of phosphine (PH3) on Jupiter and Saturn is derived using 2.5 cm−1 spectral resolution Cassini/CIRS observations. We extend the preliminary PH3 analyses on the gas giants [Irwin, P.G.J., and 6 colleagues, 2004. Icarus 172, 37-49; Fletcher, L.N., and 9 colleagues, 2007a. Icarus 188, 72-88] by (a) incorporating a wider range of Cassini/CIRS datasets and by considering a broader spectral range; (b) direct incorporation of thermal infrared opacities due to tropospheric aerosols and (c) using a common retrieval algorithm and spectroscopic line database to allow direct comparison between these two gas giants.The results suggest striking similarities between the tropospheric dynamics in the 100-1000 mbar regions of the giant planets: both demonstrate enhanced PH3 at the equator, depletion over neighbouring equatorial belts and mid-latitude belt/zone structures. Saturn's polar PH3 shows depletion within the hot cyclonic polar vortices. Jovian aerosol distributions are consistent with previous independent studies, and on Saturn we demonstrate that CIRS spectra are most consistent with a haze in the 100-400 mbar range with a mean optical depth of 0.1 at 10 μm. Unlike Jupiter, Saturn's tropospheric haze shows a hemispherical asymmetry, being more opaque in the southern summer hemisphere than in the north. Thermal-IR haze opacity is not enhanced at Saturn's equator as it is on Jupiter.Small-scale perturbations to the mean PH3 abundance are discussed both in terms of a model of meridional overturning and parameterisation as eddy mixing. The large-scale structure of the PH3 distributions is likely to be related to changes in the photochemical lifetimes and the shielding due to aerosol opacities. On Saturn, the enhanced summer opacity results in shielding and extended photochemical lifetimes for PH3, permitting elevated PH3 levels over Saturn's summer hemisphere. 相似文献
16.
Andreas F. Voegele Christofer S. Tautermann Andreas Hallbrucker Erwin Mayer Klaus R. Liedl 《Icarus》2004,169(1):242-249
Sulfurous acid (H2SO3) has never been characterized or isolated on Earth. This is caused by the unfavorable conditions for H2SO3 within Earth's atmosphere due to the high temperatures, the high water content and the oxidizing environment. Kinetic investigations by means of transition state theory showed that the half-life of H2SO3 at 300 K is 1 day but at 100 K it is increased to 2.7 billion years. Natural conditions to form H2SO3 presumably require cryogenic SO2 or SO2/H2O mixtures and high energy proton irradiation at temperatures around 100 K. Such conditions can be found on the Jupiter moons Io and Europa. Therefore, we calculated IR-spectra of H2SO3 which we compared with Galileo's spectra of Io and Europa. From the available data we surmise that H2SO3 is present on Io and probably but to a smaller extent on Europa. 相似文献
17.
The role of SO2 in the chemistry of the clouds of Venus has been investigated by deducing its mixing ratio profile in the atmosphere through millimeter wavelength interferometric measurements of the planet's limb darkening. The first zero crossing of the Venus visibility function was measured to be β0 = 0.6221 ± 0.0007 at a wavelength of 3.4 mm using a reference radius for Venus of 6100 km. This measurement constrains the amount of limb darkening and shows that the high concentrations of SO2 found in the lower atmosphere do not persist above an altitude of 42 km. Thus, a sink for SO2 exists below the level of the lowest cloud deck. 相似文献
18.
Thomas R. Hanley 《Icarus》2005,177(1):286-290
Laboratory measurements of the microwave opacity of HCl in a CO2 atmosphere have been conducted in the S (13.3 cm), X (3.6 cm), and K (1.4 cm) microwave bands at a pressure of 7.2 bar and at two different mixing ratios. The results are consistent with an opacity model employing the Van Vleck-Weisskopf lineshape applied to the published submillimeter line intensities of HCl (JPL Catalog [Pickett et al., 1998, J. Quant. Spectrosc. Rad. Trans. 60, 883-890]) and empirically fitted with a modeled parameter for CO2 broadening. Based on the deep atmospheric abundance of HCl inferred from near-infrared measurements [Dalton et al., 2000, Bull. Am. Astron. Soc. 32, 1120], the resulting modeled HCl opacity is constrained to have a small effect on the overall microwave absorption spectrum of Venus, but can be used in developing a more accurate radiative transfer model. 相似文献
19.
Chemical reactions and volatile supply through hypervelocity impacts may have played a key role for the origin and evolution of both planetary and satellite atmospheres. In this study, we evaluate the role of impact-induced N2 production from reduced nitrogen-bearing solids proposed to be contained in Titan’s crust, ammonium sulfate ((NH4)2SO4), for the replenishment of N2 to the atmosphere in Titan’s history. To investigate the conversion of (NH4)2SO4 into N2 by hypervelocity impacts, we measured gases released from (NH4)2SO4 that was exposed to hypervelocity impacts created by a laser gun. The sensitivity and accuracy of the measurements were enhanced by using an isotope labeling technique for the target. We obtained the efficiency of N2 production from (NH4)2SO4 as a function of peak shock pressure ranging from ∼8 to ∼45 GPa. Our results indicate that the initial and complete shock pressures for N2 degassing from (NH4)2SO4 are ∼10 and ∼25 GPa, respectively. These results suggest that cometary impacts on Titan (i.e., impact velocity vi > ∼8 km/s) produce N2 efficiently; whereas satellitesimal impacts during the accretion (i.e., vi < 4 km/s) produce N2 only inefficiently. Even when using the proposed small amount of (NH4)2SO4 content in the crust (∼4 wt.%) (Fortes, A.D. et al., 2007. Icarus 188, 139-153), the total amount of N2 provided through cometary impacts over 4.5 Ga reaches ∼2-6 times the present atmospheric N2 (i.e., ∼7 × 1020-2 × 1021 [mol]) based on the measured production efficiency and results of a hydrodynamic simulation of cometary impacts onto Titan. This implies that cometary impacts onto Titan’s crust have the potential to account for a large part of the present N2 through the atmospheric replenishment after the accretion. 相似文献
20.
Photolysis of NH3 in the presence of CH4 with a 185-nm light source results in the generation of hot hydrogen atoms that abstract hydrogen from the CH4 to produce CH3·. Subsequent reactions of CH3· and NH2· give hydrocarbons, CH3NH2, and HCN. The extent of reaction of CH4 was measured by the ratio of the moles of CH4 reacted per mole of NH3 decomposed (). This ratio increases with diminishing NH3 pressure at constant CH4 pressure but it remains constant if . The ratio is independent of temperature in the range 156–298° K, suggesting that hot hydrogen atoms were responsible for the reaction of CH4. This postulate was confirmed by the observation that this reaction was quenched when H2 or SF6 was added to the reaction mixture. 相似文献