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28 records · Page 2
All sourcesNASA NTRSDOE OSTI
NASA NTRS1995

The Atmospheric Lifetime Experiment and the Global Atmospheric Gas Experiment (ALE/GAGE)

The ALE/GAGE project was designed to determine the global atmospheric lifetimes of the chlorofluorocarbons CCl3F and CCl2F2 (F-11 and F-12), which had been identified as the main gases that cause stratospheric ozone depletion. The experimental procedures also provided the concentrations of CH3CCl3, CCl4 and N2O. The extended role of the project was to evaluate the mass balances of these gases as well. Methylchloroform (CH3CCl3) serves as a tracer of average atmospheric OH concentrations and hence the oxidizing capacity of the atmosphere. Nitrous oxide (N2O) is a potent greenhouse gas and can also deplete the ozone layer. Measurements of these gases were taken with optimized instruments in the field at a frequency of about 1 sample/hr. Toward the end of the present project methane measurements were added to the program. The final report deals with the research of the Oregon Graduate Institute (OGI) as part of the ALE/GAGE program between 4/1/1988 and 1/31/1991. The report defines the scope of the OGI project, the approach, and the results.

Rasmussen, R. A.↗
NASA NTRS1993

Measurements of halogenated organic compounds near the tropical tropopause

The amount of organic chlorine and bromine entering the stratosphere have a direct influence on the magnitude of chlorine and bromine catalyzed ozone losses. Twelve organic chlorine species and five organic bromine species were measured from 12 samples collected near the tropopause between 23.8 deg N and 25.3 deg N during AASE 2. The average mixing ratios of total organic chlorine and total organic bromine were 3.50 +/- 0.06 ppbv and 21.1 +/- 0.8 pptv, respectively. CH3Cl represented 15.1% of the total organic chlorine, with CFC 11 (CCl3F) and CFC 12 (CCl2F2) accounting for 22.6% and 28.2%, respectively, with the remaining 34.1% primarily from CCl4, CH3CCl3, and CFC 113 (CCl2FCClF2). CH3Br represented 54% of the total organic bromine. The 95% confidence intervals of the mixing ratios of all but four of the individual compounds were within the range observed in low and mid-latitude mid-troposphere samples. The four compounds with significantly lower mixing ratios at the tropopause were CHCl3, CH2Cl2, CH2Br2, and CH3CCl3. The lower mixing ratios may be due to entrainment of southern hemisphere air during vertical transport in the tropical region and/or to exchange of air across the tropopause between the lower stratosphere and upper troposphere.

Schauffler, S. M.↗
NASA NTRS1994

Measurement of the absorption cross-sections of CFC-11 at conditions representing various model atmospheres

Absorption cross-sections, K(sub V)(/(cm)(atm)), have been measured in the 9.2 and 11.8 micrometer bands of CFC-11 (CCl3F) using a high-resolution Fourier transform spectrometer. Temperature and total (N2-broadening) pressure have been varied to obtain results at conditions representative of the atmosphere. The measured absolute intensities (in units of 10(exp -17) cm/molecule of the 9.2 and 11.8 micrometer bands are 2.591 +/- 0.013 and 6.974 +/- 0.038, respectively.

Li, Zhenhua↗
NASA NTRS1996

On the Assessment and Uncertainty of Atmospheric Trace Gas Burden Measurements with High Resolution Infrared Solar Occultation Spectra from Space by the ATMOS Experiment

The Atmospheric Trace Molecule Spectroscopy (ATMOS) instrument is a high resolution Fourier transform spectrometer that measures atmospheric composition from low Earth orbit with infrared solar occultation sounding in the limb geometry. Following an initial flight in 1985, ATMOS participated in the Atmospheric Laboratory for Applications and Science (ATLAS) 1, 2, and 3 Space Shuttle missions in 1992, 1993, and 1994 yielding a total of 440 occultation measurements over a nine year period. The suite of more than thirty atmospheric trace gases profiled includes CO2, O3, N2O, CH4, H2O, NO, NO2, HNO3, HCl, HF, ClONO2, CCl3F, CCl2F2, CHF2Cl, and N2O5. The analysis method has been revised throughout the mission years culminating in the 'version 2' data set. The spectroscopic error analysis is described in the context of supporting the precision estimates reported with the profiles; in addition, systematic uncertainties assessed from the quality of the spectroscopic database are described and tabulated for comparisons with other experiments.

Abrams, M. C.↗
NASA NTRS1993

Measurements of Halogenated Organic Compounds near the Tropical Tropopause

The amount of organic chlorine and bromine entering the stratosphere have a direct influence on the magnitude of chlorine and bromine catalyzed ozone losses. Twelve organic chlorine species and five organic bromine species were measured from 12 samples collected near the tropopause between 23.8 deg N and 25.3 deg N during AASE 2. The average mixing ratios of total organic chlorine and total organic bromine were 3.50 +/- 0.06 ppbv and 21.1 +/- 0.8 pptv, respectively. CH3Cl represented 15.1% of the total organic chlorine, with CFC 11 (CCl3F) and CFC 12 (CCl2F2) accounting for 22.6% and 28.2%, respectively, with the remaining 34.1% primarily from CCl4, CH3CCl3, and CFC 113 (CCl2FCClF2). CH3Br represented 54% of the total organic bromine. The 95% confidence intervals of the mixing ratios of all but four of the individual compounds were within the range observed in low and mid-latitude midtroposphere samples. The four compounds with significantly lower mixing ratios at the tropopause were CHCl3, CH2Cl2, CH2Br2, and CH3CCl3. The lower mixing ratios may be due to entrainment of southern hemisphere air during vertical transport in the tropical region and/or to exchange of air across the tropopause between the lower stratosphere and upper troposphere.

Schauffler, S. M.↗
NASA NTRS1996

Bulk Properties of Isentropic Mixing into the Tropics in the Lower Stratosphere

Timescales for mixing of midlatitude air into the tropical lower stratosphere are deduced from observations of long-lived tracers N2O and CCl3F. Bulk mixing between tropical and midlatitude regions is assumed to be isentropic and relatively slow compared with local mixing within each region. The mean value of the mixing timescale ranges from 12 to 18 months near 20 km. There is a tendency for shorter mixing times at higher and lower altitudes, although vertical profiles of mixing cannot be definitively established by the data. A more robust quantity is given by the fraction of midlatitude air entrained into the tropical upwelling region. Implied mixing fractions exceed 50% above 22 km.

Minschwaner, K.↗
NASA NTRS1998

Distribution of Halon-1211 in the Upper Troposphere and Lower Stratosphere and the 1994 Total Bromine Budget

We report here on the details of the first, in situ, real-time measurements of H-1211 (CBrClF2) and sulfur hexafluoride (SF6) mixing ratios in the stratosphere up to 20 km. Stratospheric air was analyzed for these gases and others with a new gas chromatograph, flown aboard a National Aeronautics and Space Administration ER-2 aircraft as part of the Airborne Southern Hemisphere Ozone Experiment/Measurements for Assessing the Effects of Stratospheric Aircraft mission conducted in 1994. The mixing ratio of SF6, with its nearly linear increase in the troposphere, was used to estimate the mean age of stratospheric air parcels along the ER-2 flight path. Measurements of H-1211 and mean age estimates were then combined with simultaneous measurements of CFC-11 (CCl3F), measurements of brominated compounds in stratospheric whole air samples, and records of tropospheric organic bromine mixing ratios to calculate the dry mixing ratio of total bromine in the lower stratosphere and its partitioning between organic and inorganic forms. We estimate that the organic bromine-containing species were almost completely photolyzed to inorganic species in the oldest air parcels sampled. Our results for inorganic bromine are consistent with those obtained from a photochemical, steady state model for stratospheric air parcels with CFC- I I mixing ratios greater than 150 ppt. For stratospheric air parcels with CFC-11 mixing ratios less than 50 ppt (mean age greater than or equal to 5 years) we calculate inorganic bromine mixing ratios that are approximately 20% less than the photo-chemical, steady state model. There is a 20% reduction in calculated ozone loss resulting from bromine chemistry in old air relative to some previous estimates as a result of the lower bromine levels.

Wamsley, P. R.↗
NASA NTRS2003

Advanced Global Atmospheric Gases Experiment (AGAGE): MIT Contribution

We describe in detail the instrumentation and calibrations used in the ALE, GAGE and AGAGE experiments and present a history of the majority of the anthropogenic ozone- depleting and climate-forcing gases in air based on these experiments. Beginning in 1978, these three successive automated high frequency in-situ experiments have documented the long-term behavior of the measured concentrations of these gases over the past twenty years, and show both the evolution of latitudinal gradients and the high frequency variability due to sources and circulation. We provide estimates of the long-term trends in total chlorine contained in long- lived halocarbons involved in ozone depletion. We summarize interpretations of these measurements using inverse methods to determine trace gas lifetimes and emissions. Finally, we provide a combined observational and modeled reconstruction of the evolution of chlorocarbons by latitude in the atmosphere over the past sixty years which can be used as boundary conditions for interpreting trapped air in glaciers and oceanic measurements of chlorocarbon tracers of the deep oceanic circulation. Some specific conclusions are: (a) International compliance with the Montreal Protocol is so far resulting in chlorofluorocarbon and chlorocarbon mole fractions comparable to target levels, (b) Mole fractions of total chlorine contained in long-lived halocarbons (CCl2F2, CCl3F, CH3CCl3, CCl4, CHClF2, CCl2FCClF2, CH3Cl, CH2Cl2, CHCl3, CCl2=CCl2) in the lower troposphere reached maximum values of about 3.6 ppb in 1993 and are beginning to slowly decrease in the global lower atmosphere, (c) The chlorofluorocarbons have atmospheric lifetimes consistent with destruction in the stratosphere being their principal removal mechanism, (d) Multi-annual variations in chlorofluorocarbon and chlorocarbon emissions deduced from ALUGAGWAGAGE data are consistent approximately with variations estimated independently from industrial production and sales data where available (CCl2F2 (CFC-12) and CCl2FCClF2 (CFC-113) show the greatest discrepancies), (e) The mole fractions of the hydrochlorofluorocarbons and hydrofluorocarbons, which are replacing the regulated halocarbons, are rising very rapidly in the atmosphere but, with the exception of the much longer manufactured CHClF2 (HCFC-22), they are not yet at levels sufficient to contribute significantly to atmospheric chlorine loading. These replacement species could in the future provide independent estimates of the global weighted-average OH concentration provided their industrial emissions are accurately documented, (f) In the future, analysis of pollution events measured using high frequency in-situ measurements of chlorofluorocarbons and their replacements may enable emission estimates at the regional level which, together with industrial end-use data, are of sufficient accuracy to be capable of identifying regional non-compliance with the Montreal Protocol.

Kurylo, Michael↗
NASA NTRS2009

First Global Observations of Atmospheric COClF from the Atmospheric Chemistry Experiment Mission

Carbonyl chlorofluoride (COClF) is an important reservoir of chlorine and fluorine in the Earth's atmosphere. Satellite-based remote sensing measurements of COClF, obtained by the Atmospheric Chemistry Experiment (ACE) for a time period spanning February 2004 through April 2007, have been used in a global distribution study. There is a strong source region for COClF in the tropical stratosphere near 27 km. A layer of enhanced COClF spans the low- to mid-stratosphere over all latitudes, with volume mixing ratios of 40-100 parts per trillion by volume, largest in the tropics and decreasing toward the poles. The COClF volume mixing ratio profiles are nearly zonally symmetric, but they exhibit a small hemispheric asymmetry that likely arises from a hemispheric asymmetry in the parent molecule CCl3F. Comparisons are made with a set of in situ stratospheric measurements from the mid-1980s and with predictions from a 2-D model.

Fu, Dejian↗
NASA NTRS2009

Appendix C: First Global Observations of Atmospheric COClF from the Atmospheric Chemistry Experiment Mission

Carbonyl chlorofluoride (COCIF) is an important reservoir of chlorine and Fluorine in the Earth's atmosphere. Satellite-based remote sensing measurements of COCIF, obtained by Received in revised form the Atmospheric Chemistry Experiment (ACE) for a time period spanning February 2004 through April 2007, have been used in a global distribution study. There is a strong Accepted 18 February 2009 source region for COCIF in the tropical stratosphere near 27 km. A layer of enhanced COCIF spans the low- to mid-stratosphere over all latitudes, with volume mixing ratios of 40-100 parts Per trillion by volume, largest in the tropics and decreasing toward the poles. The COCIF volume mixing ratio profiles are nearly zonally symmetric, but they exhibit a small hemispheric asymmetry that likely arises from a hemispheric asymmetry in the parent molecule CCl3F. Comparisons are made with a set of in situ stratospheric measurements from the mid-1980s and with predictions from a 2-D model.

Fu, Djian↗