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At least 163 records · Page 9

Vertical transport rates in the statosphere in 1993 from observations of CO2, N2O, and CH4

Measurements of CO2, N2O, and CH4 are analyzed to define hemispheric average vertical exchange rates in the lower stratosphere from November 1992 to October 1993. Effective vertical diffusion coefficients were small in summer, less than or equal to 1 sq m/s at altitudes below 25 km; values were similar near the tropopause in winter, but increased markedly with altitude. The analysis suggests possible longer residence times for exhaust from stratospheric aircraft, and more efficient transport from 20 km to the middle stratosphere, than predicted by many current models. Seasonally-resolved measurements of stratospheric CO2 and N2O provide significant new constraints on rates for global-scale vertical transport.

Wofsy, Steven C.↗

Seasonal Variations of Water Vapor in the Lower Stratosphere Inferred from ATMOS/ATLAS-3 Measurements of H2O and CH4

Stratospheric measurements of H2O and CH4 by the Atmospheric Trace Molecule Spectroscopy (ATMOS) Fourier transform spectrometer on the ATLAS-3 shuttle flight in November 1994 have been examined to investigate the altitude and geographic variability of H2O and the quantity H = (H2O + 2CH4) in the tropics and at mid-latitudes (8 to 49 deg N) in the northern hemisphere. The measurements indicate an average value of 7.24 +/- 0.44 ppmv for H between altitudes of about 18 to 35 km, corresponding to an annual average water vapor mixing ratio of 3.85 +/- 0.29 ppmv entering the stratosphere. The H2O vertical distribution in the tropics exhibits a wave-like structure in the 16- to 25-km altitude range, suggestive of seasonal variations in the water vapor transported from the troposphere to the stratosphere. The hygropause appears to be nearly coincident with the tropopause at the time of observations. This is consistent with the phase of the seasonal cycle of H2O in the lower stratosphere, since the ATMOS observations were made in November when the H2O content of air injected into the stratosphere from the troposphere is decreasing from its seasonal peak in July-August.

Abbas, M. M.↗

Seasonal Variations of Water Vapor in the Lower Stratosphere Inferred from ATMOS/ATLAS-3 Measurements of H2O and CH4

Stratospheric measurements of H2O and CH4 by the Atmospheric Trace Molecule Spectroscopy (ATMOS) Fourier transform spectrometer on the ATLAS-3 shuttle flight in November 1994 have been examined to investigate the altitude and geographic variability of H2O and the quantity H = (H2O + 2CH4) in the tropics and at mid-latitudes (8 to 49 deg N) in the northern hemisphere. The measurements indicate an average value of 7.24 plus or minus 0.44 ppmv for H between altitudes of about 18 to 35 km, corresponding to an annual average water vapor mixing ratio of 3.85 plus or minus 0.29 ppmv entering the stratosphere. The H2O vertical distribution in the tropics exhibits a wave-like structure in the 16- to 25-km altitude range, suggestive of seasonal variations in the water vapor transported from the troposphere to the stratosphere. The hygropause appears to be nearly coincident with the tropopause at the time of observations. This is consistent with the phase of the seasonal cycle of H2O in the lower stratosphere, since the ATMOS observations were made in November when the H2O content of air injected into the stratosphere from the troposphere is decreasing from its seasonal peak in July - August.

Abbas, M. M.↗

Vertical Transport Rates in the Stratosphere in 1993 from Observations of CO2, N2O and CH4

Measurements of CO2, N2O and CH4 are analyzed to define hemispheric average vertical exchange rates in the lower stratosphere from November 1992 to October 1993. Effective vertical diffusion coefficients were small in summer, less than or equal to 1 m(exp 2)/sec at altitudes below 25 km; values were similar near the tropopause in winter, but increased markedly with altitude. The analysis suggests possibly longer residence times for exhaust from stratospheric aircraft, and more efficient transport from 20 km to the middle stratosphere, than predicted by many current models. Seasonally-resolved measurements of stratospheric CO2 and N2O provide significant new constraints on rates for global-scale vertical transport.

Wofsy, Steven C.↗

Correlations of Stratospheric Abundances of CH4 and N2O Derived from ATMOS Measurements

Atmospheric Trace MOlecule Spectroscopy (ATMOS) measurements made over a wide range of altitudes and latitudes demonstrate compact correlations between mixing ratios of CH, and N,O. Tight but distinct correlations are observed for the tropics, the springtime Arctic vortex, and the extra-tropics/extra-vortex regions, indicating dynamical isolation between these regions. Little variability is apparent in correlations between CH4 and N20 from measurements made in different years (1992, 1993, and 1994), seasons (March/April and November), and hemispheres.

Rinsland, C. P.↗

Stratospheric N2O5, CH4, and N2O Profiles from IR Solar Occultation Spectra

Stratospheric volume mixing ratio profiles of N2O5, CH4, and N2O have been retrieved from a set of 0.052/ cm resolution (FWHM) solar occultation spectra recorded at sunrise during a balloon flight from Aire sur I'Adour, France (44 deg N latitude) on 12 October 1990. The N2O5 results have been derived from measurements of the integrated absorption by the 1246/ cm band. Assuming a total intensity of 4.32 x 10(exp 17)cm(exp -1) molecule sq cm(exp -2) independent of temperature, the retrieved N2O5 volume mixing ratios in ppbv (parts per billion by volume, 10(exp -9)), interpolated to 2 km height spacings, are 1.64 +/- 0.49 at 37.5 km, 1.92 +/- 0.56 at 35.5 km, 2.06 +/- 0.47 at 33.5 km, 1.95 +/- 0.42 at 31.5 km, 1.60 +/- 0.33 at 29.5 km, 1.26 +/- 0.28 at 27.5 km, and 0.85 +/- 0.20 at 25.5 km. Error bars indicate the estimated I-sigma uncertainty including the error in the total band intensity (+/- 20% has been assumed). The retrieved profiles are compared with previous measurements and photochemical model results.

Peyeret, C. Camy↗

BOREAS TF-1 SSA-OA Weekly Tower CH4 and N2O Flux

The BOREAS TF-1 team collected various trace gas and energy flux data in its efforts to characterize the temporal energy and gas exchanges that occurred over the SSA-OA site. This data set contains methane (CH4) and nitrous oxide (N2O) fluxes that were measured at the BOREAS SSA-OA site. These fluxes were measured from 16-Apr to 16-Sep-1994. The data were averaged to weekly values and are available in tabular ASCII files.

Thurtell, George↗

BOREAS TGB-3 CH4 and CO2 Chamber Flux Data over NSA Upland Sites

The BOReal Ecosystem-Atmosphere Study Trace Gas Biogeochemistry (BOREAS TGB-3) team collected methane and carbon dioxide (CH4, CO2) chamber flux measurements at the Northern Study Area (NSA) Fen, Old Black Spruce (OBS), Young Jack Pine (YJP), and auxiliary sites along Gillam Road and the 1989 burn site. Gas samples were extracted from chambers and analyzed at the NSA lab facility approximately every 7 days during May to September 1994 and June to October 1996. The data are provided in tabular ASCII files.

Savage, Kathleen↗

BOREAS TGB-5 CO2, CH4 and CO Chamber Flux Data Over the NSA

The BOReal Ecosystem-Atmosphere Study Trace Gas Biogeochemistry (BOREAS TGB-5) team collected a variety of trace gas concentration and flux measurements at several NSA sites. This data set contains carbon dioxide (CO2), methane (CH4), and carbon monoxide (CO) chamber flux measurements conducted in 1994 at upland forest sites that experienced stand-replacement fires. These measurements were acquired to understand the impact of fires on soil biogeochemistry and related changes in trace gas exchange in boreal forest soils. Relevant ancillary data, including data concerning the soil temperature, solar irradiance, and information from nearby un-burned control sites, are included to provide a basis for modeling the regional impacts of fire and climate changes on trace gas biogeochemistry. The data are provided in tabular ASCII files.

Burke, Roger↗

BOREAS TF-4 CO2 and CH4 Soil Profile Data from the SSA

The BOReal Ecosystem-Atmosphere Study Tower Flux (BOREAS TF-4) team measured distributions of carbon dioxide (CO2) and methane (CH4) concentrations for the upper 5 m of soil and unsaturated zone at the mature stand, upper 6 m at the 20-year-old stand, and the upper 1 m at the 8-year-old stand and clear cut area at the BOREAS Southern Study Area (SSA) during August 1993 to March 1995. Particle size and carbon content of the unsaturated deposits, precipitation, soil temperature and moisture, carbon and oxygen isotopes of soil CO2, and soil water chemistry are also presented. The data are stored in tabular ASCII files.

Striegl, Robert↗

BOREAS TGB-1/TGB-3 CH4 Chamber Flux Data over the NSA Fen

The BOREAS TGB-3 team collected methane (CH4) chamber flux measurements at the NSA fen site during May-September 1994 and June-October 1996. Gas samples were extracted approximately every 7 days from chambers and analyzed at the NSA lab facility. The data are provided in tabular ASCII files.

Bubier, Jill L.↗

BOREAS TGB-1 NSA CH4 and CO2 Chamber Flux Data

The BOREAS TGB-1 team made methane (CH4) and carbon dioxide (CO2) dark chamber flux measurements at the NSA-OJP, NSA-OBS, NSA-BP, and NSA-YJP sites from 16-May-1994 through 13-Sep-1994. Gas samples were extracted approximately every 7 days from dark chambers and analyzed at the NSA lab facility. The data are provided in tabular ASCII files.

Hall, Forrest G.↗

The Effects of Flame Structure on Extinction of CH4-O2-N2 Diffusion Flames

The effects of flame structure on the extinction limits of CH4-O2-N2 counterflow diffusion flames were investigated experimentally and numerically by varying the stoichiometric mixture fraction Z(sub st), Z(sub st) was varied by varying free-stream concentrations, while the adiabatic flame temperature T(sub ad) was held fixed by maintaining a fixed amount of nitrogen at the flame. Z(sub st) was varied between 0.055 (methane-air flame) and 0.78 (diluted- methane-oxygen flame). The experimental results yielded an extinction strain rate K(sub ext) of 375/s for the methane-air flame, increasing monotonically to 1042/s for the diluted-methane-oxygen flame. Numerical results with a 58-step Cl mechanism yielded 494/s and 1488/s, respectively. The increase in K(sub ext) with Z(sub st) for a fixed T(sub ad) is explained by the shift in the O2 profile toward the region of maximum temperature and the subsequent increase in rates for chain-branching reactions. The flame temperature at extinction reached a minimum at Z(sub st) = 0.65, where it was 200 C lower than that of the methane-air flame. This significant increase in resistance to extinction is seen to correspond to the condition in which the OH and O production zones are centered on the location of maximum temperature.

Du, J.↗

Mean Ages of Stratospheric Air Derived From in Situ Observations of CO2, CH4, and N2O

Accurate mean ages for stratospheric air have been derived from a spatially and temporally comprehensive set of in situ observations of CO2, CH4, and N2O obtained from 1992 to 1998 from the NASA ER-2 aircraft and balloon flights. Errors associated with the tropospheric CO2 seasonal cycle and interannual variations in the CO2 growth rate are less than 0.5 year throughout the stratosphere and less than 0.3 year for air older than 2 years (N2O less than 275 ppbv), indicating that the age spectra are broad enough to attenuate these influences over the time period covered by these observations. The distribution of mean age with latitude and altitude provides detailed, quantitative information about the general circulation of the stratosphere. At 20 km, sharp meridional gradients in the mean age are observed across the subtropics. Between 20 and 30 km, the average difference in mean age between the tropics and midlatitudes is approximately 2 years, with slightly smaller differences at higher and lower altitudes. The mean age in the midlatitude middle stratosphere (approx. 25-32 km) is relatively constant with respect to altitude at 5 plus or minus 0.5 years. Comparison with earlier balloon observations of CO2 dating back to the 1970s indicates that the mean age of air in this region has remained within 11 year of its current value over the last 25 years. A climatology of mean age is derived from the observed compact relationship between mean age and N2O. These characteristics of the distribution of mean age in the stratosphere will serve as critically needed diagnostics for models of stratospheric transport.

Andrews, A. E.↗

The Dissociation Energies of CH4 and C2H2 Revisited

The bond dissociation energies of CH4 and C2H2 and their fragments are investigated using basis set extrapolations and high levels of correlation. The computed bond dissociation energies (D(sub e)) are accurate to within 0.2 kcal/mol. The agreement with the experimental (D(sub 0)) values is excellent if we assume that the zero-point energy of C2H is 9.18 kcal/mol. The effect of core (1s) correlation on the bond dissociation energies of C-H bonds is shown to vary from 0.2 to 0.7 kcal/mol and that for C-C bonds varies from 0.4 to 2.2 kcal/mol.

Partridge, Harry↗

A Time-Dependent Quantum Dynamics Study of the H2 + CH3 yields H + CH4 Reaction

We present a time-dependent wave-packet propagation calculation for the H2 + CH3 yields H + CH4 reaction in six degrees of freedom and for zero total angular momentum. Initial state selected reaction probability for different initial rotational-vibrational states are presented in this study. The cumulative reaction probability (CRP) is obtained by summing over initial-state-selected reaction probability. The energy-shift approximation to account for the contribution of degrees of freedom missing in the 6D calculation is employed to obtain an approximate full-dimensional CRP. Thermal rate constant is compared with different experiment results.

Wang, Dunyou↗

Remote-Raman and Micro-Raman Studies of Solid CO2, CH4, Gas Hydrates and Ice

It is well known that on Mars CO2 is the principal constituent of the thin atmosphere and on a seasonal basis CO2 snow and frost coats the polar caps. Also over 25% of the Martian atmosphere freezes out and sublimes again each year. The Mars Odyssey Emission Imaging system (THEMIS) has discovered water ice exposed near the edge of Mars southern perennials cap. In recent years, it has been suggested that in Martian subsurface CO2 may exist as gas hydrate (8CO2 + 44 H2O) with melting temperature of 10C. Since the crust of Mars has been stable for enough time there is also a possibility that methane formed by magmatic processes and/or as a byproduct of anaerobic deep biosphere activity to have raised toward the planet s surface. This methane would have been captured and stored as methane hydrate, which concentrates methane and water. Determination of abundance and distribution of these ices on the surface and in the near surface are of fundamental importance for understanding Martian atmosphere, and for future exploration of Mars. In this work, we have evaluated feasibility of using remote Raman and micro-Raman spectroscopy as potential nondestructive and non-contact techniques for detecting solid CO2, CH4 gas, and gas hydrates as well as water-ice on planetary surfaces.

Sharma, S. K.↗

Argus: a new instrument for the measurement of the stratospheric dynamical tracers, N2O and CH4

We describe here a new instrument for the simultaneous, in situ measurement of the stratospheric tracer molecules, nitrous oxide (N2O) and methane (CH4). Argus is unique in its small size making it well suited for limited payload atmospheric research platforms. Argus employs second harmonic spectroscopy using tunable lead-salt diode lasers emitting in the mid-infrared. We first explain the Argus design philosophy followed by detailed descriptions of the instrument's optical, mechanical, and thermal sub-systems. Argus employs an in-flight calibration system providing real time calibrations and tightly constrained uncertainty estimates of the returned data. Data analysis is carried out using non-linear least-squares model fits to the acquired second harmonic spectra. A sampling of Argus data acquired on a recent stratospheric research campaign in the Arctic winter is presented.

Methane/analysis↗