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See detailNorthern and southern hemisphere ground-based infrared spectroscopic measurements of tropospheric carbon monoxide and ethane
Rinsland, C. P.; Jones, N. B.; Connor, B. J. et al

in Journal Of Geophysical Research. Atmospheres (1998), 103(D21), 28197-28217

Time series of CO and C2H6 measurements have been derived from high-resolution infrared solar spectra recorded in Lauder, New Zealand (45.0 degrees S, 169.7 degrees E, altitude 0.37 km), and at the U.S ... [more ▼]

Time series of CO and C2H6 measurements have been derived from high-resolution infrared solar spectra recorded in Lauder, New Zealand (45.0 degrees S, 169.7 degrees E, altitude 0.37 km), and at the U.S. National Solar Observatory (31.9 degrees N, 111.6 degrees W, altitude 2.09 km) on Kitt Peak. Lauder observations were obtained between July 1993 and November 1997, while the Kitt Peak measurements were recorded between May 1977 and December 1997. Both databases were analyzed with spectroscopic parameters that included significant improvements for C2H6 relative to previous studies. Target CO and C2H6 lines were selected to achieve similar vertical samplings based on averaging kernels. These calculations show that partial columns from layers extending from the surface to the mean tropopause and from the mean tropopause to 100 km are nearly independent. Retrievals based on a semiempirical application of the Rodgers optimal estimation technique are reported for the lower laver, which has a broad maximum in sensitivity in the upper troposphere. The Lauder CO and C2H6 partial columns exhibit highly asymmetrical seasonal cycles with minima in austral autumn and sharp peaks in austral spring. The spring maxima are the result of tropical biomass burning emissions followed by deep convective vertical transport to the upper troposphere and long-range horizontal transport. Significant year-to-year variations are observed for both CO and C2H6, but the measured trends, (+0.37 +/- 0.57)% yr(-1) and (-0.64 +/- 0.79)% yr(-1), 1 sigma, respectively, indicate no significant long-term changes. The Kitt Peak data also exhibit CO and C2H6 seasonal variations in the lower layer with trends equal to (-0.27 +/- 0.17)% yr(-1) and (-1.20 +/- 0.35')% yr(-1), 1 sigma, respectively. Hence a decrease in the Kitt Peak tropospheric C2H6 column has been detected, though the CO trend is not significant. Both measurement sets are compared with previous observations, reported trends, and three-dimensional model calculations. [less ▲]

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See detailGround-based infrared solar spectroscopic measurements of carbon monoxide during 1994 Measurement of Air Pollution From Space flights
Pougatchev, N. S.; Jones, N. B.; Connor, B. J. et al

in Journal Of Geophysical Research. Atmospheres (1998), 103(D15), 19317-19325

Results of the comparison of carbon monoxide ground-based infrared solar spectroscopic measurements with data obtained during 1994 Measurement of Air Pollution From Space (MAPS) flights are presented ... [more ▼]

Results of the comparison of carbon monoxide ground-based infrared solar spectroscopic measurements with data obtained during 1994 Measurement of Air Pollution From Space (MAPS) flights are presented. Spectroscopic measurements were performed correlatively with April and October MAPS flights by nine research groups from Belgium, Canada, Germany, Japan, New Zealand, Russia, and the United States. Characterization of the techniques and error analysis were performed. The role of the CO a priori profile used in the retrieval was estimated. In most cases an agreement between spectroscopic and MAPS data is within estimated MAPS accuracy of +/-10%. [less ▲]

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See detailThe current budjet of NOy above the Jungfraujoch as derived from IR Solar Observations.
Demoulin, Philippe ULg; Mahieu, Emmanuel ULg; Zander, Rodolphe ULg et al

in Air Pollution Research Report Nr 66 (1998). (1997)

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See detailRetrieval of ozone vertical column amounts from ground-based high resolution infrared solar spectra
Hamdouni, A.; Barbe, Alain; Demoulin, Philippe ULg et al

in Journal of Quantitative Spectroscopy & Radiative Transfer (1997), 57(1), 11-22

Good infrared spectral regions to retrieve accurately the vertical column amount of ozone from ground observations are proposed. Their selection was based on studies of the influence of spectroscopic ... [more ▼]

Good infrared spectral regions to retrieve accurately the vertical column amount of ozone from ground observations are proposed. Their selection was based on studies of the influence of spectroscopic (frequencies, half-widths, intensities) as well as geophysical parameters (volume mixing ratios, temperature profiles) with a particular attention for temperature. The results, obtained in three different spectral regions, with a realistic T-profile are very consistent. [less ▲]

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See detailTotal vertical column abundances of atmospheric gases derived from IR remote solar observations made at the Jungfraujoch Station.
Zander, Rodolphe ULg; Demoulin, Philippe ULg; Mahieu, Emmanuel ULg et al

in Hov, O. (Ed.) Transport and Chemical Transformation of Pollutants in the Troposphere. (1997)

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See detailObserved trends in total vertical column abundances of atmospheric gases from IR solar spectra recorded at the Jungfraujoch
Mahieu, Emmanuel ULg; Zander, Rodolphe ULg; Delbouille, Luc et al

in Journal of Atmospheric Chemistry (1997), 28(1-3), 227-243

Since 1984, about 15 000 high quality infrared solar spectra have been recorded with state-of-the-art grating and Fourier transform spectrometers at the International Scientific Station of the ... [more ▼]

Since 1984, about 15 000 high quality infrared solar spectra have been recorded with state-of-the-art grating and Fourier transform spectrometers at the International Scientific Station of the Jungfraujoch, Switzerland. Nonlinear least squares spectral curve fitting of selected microwindows containing isolated and well characterized lines of 20 telluric gases have allowed to retrieve their total vertical column abundances above the station, leading to observational data bases essential to derive long- and short-term changes experienced by these species during the last 12 years. In this paper, we focus on atmospheric gases of particular interest within the context of the EUROTRACTOR (Tropospheric Ozone Research) project; secular evolution as well as seasonal cycles of the minor constituents CH4, CO and of the trace gases C2H6, OCS, C2H2, HCN and H2CO are reported and discussed. The long-lived N2O is included as a tracer of the dynamic activity of the atmosphere. [less ▲]

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See detailOn the use of HF as a reference for the comparison of stratospheric observations and models
Chipperfield, M. P.; Burton, M.; Bell, W. et al

in Journal of Geophysical Research (1997), 102(11D), 12901-12919

Hydrogen fluoride (HF) is often used as a simple reference for other column observations of chemically active stratospheric species. However, seasonal and shorter timescale variations in column HF make ... [more ▼]

Hydrogen fluoride (HF) is often used as a simple reference for other column observations of chemically active stratospheric species. However, seasonal and shorter timescale variations in column HF make its use as a reference more complicated. In this paper we characterize the expected magnitude of these variations in HF, and variations of ratio quantities involving HF, using a two-dimensional (2-D) photochemical model and two versions of a three-dimensional (3-D) transport model. The 2-D model predicts that the column ratios HNO3/HF and HCl/HF increase from midlatitudes to the tropics, although this is very sensitive to HCl and HNO3 abundances in the tropical upper troposphere. Seasonal variations in vertical motion modifys the predicted ratios; for example, wintertime descent at high latitudes decreases HCl/HF. The ratio HNO3/HF at high latitudes is strongly modified by seasonal variations in the chemical partitioning of the odd nitrogen (NOy) species. We compare these model predictions with ground-based Fourier transform infrared spectroscopy (FTIR) observations of HF along with HCl, ClONO2 and HNO3 obtained at eight northern hemisphere sites between October 1994 and July 1995. We investigate quantitatively how HF can be used as a tracer to follow the evolution of observations at a single station and to intercompare results from different stations or with photochemical models. The magnitude of the 3-D model HF column agrees well with the observations, except on some occasions at high latitudes, giving indirect support for the important role of COF2 in the stratospheric inorganic fluorine budget. The observed day-to-day variability in the column ratios HCl/HF and HNO3/HF is much larger at high latitudes. This variability is reproduced in the 3-D models and is due to horizontal motion. Short timescale vertical displacement of the species profiles is estimated to have a small effect on the column ratios. In particular, we analyze the usefulness of the observed column ratio (ClONO2 + HCl)/HF as an indicator for chlorine activation. Current measurement uncertainties limit the degree of activation which can be unambiguously detected using this observed quantity, but we can determine that chlorine-activated air was observed above Aberdeen (58 degrees N) on 6 days in late January 1995. [less ▲]

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See detailThe 1994 northern midlatitude budget of stratospheric chlorine derived from ATMOS/ATLAS-3 observations
Zander, Rodolphe ULg; Mahieu, Emmanuel ULg; Gunson, M. R. et al

in Geophysical Research Letters (1996), 23(17), 2357-2360

Volume mixing ratio (VMR) profiles of the chlorine-bearing gases HCl, ClONO2, CCl3F, CCl2F2, CHClF2, CCl4, and CH3Cl have been measured between 3 and 49 degrees northern- and 65 to 72 degrees southern ... [more ▼]

Volume mixing ratio (VMR) profiles of the chlorine-bearing gases HCl, ClONO2, CCl3F, CCl2F2, CHClF2, CCl4, and CH3Cl have been measured between 3 and 49 degrees northern- and 65 to 72 degrees southern latitudes with the Atmospheric Trace MOlecule Spectroscopy (ATMOS) instrument during the ATmospheric Laboratory for Applications and Science (ATLAS)-3 shuttle mission of 3 to 12 November 1994. A subset of these profiles obtained between 20 and 49 degrees N at sunset, combined with ClO profiles measured by the Millimeter-wave Atmospheric Sounder (MAS) also from aboard ATLAS-3, measurements by balloon for HOCl, CH3CCl3 and C2Cl3F3, and model calculations for COClF indicates that the mean burden of chlorine, Cl-TOT, was equal to (3.53 +/- 0.10) ppbv (parts per billion by volume), 1-sigma, throughout the stratosphere at the time of the ATLAS 3 mission. This is some 37% larger than the mean 2.58 ppbv value measured by ATMOS within the same latitude zone during the Spacelab 3 flight of 29 April to 6 May 1985, consitent with an exponential growth rate of the chlorine loading in the stratosphere equal to 3.3%/yr or a linear increase of 0.10 ppbv/yr over the Spring-1985 to Fall-1994 time period. These findings are in agreement with both the burden and increase of the main anthropogenic Cl-bearing source gases at the surface during the 1980s, confirming that the stratospheric chlorine loading is primarily of anthropogenic origin. [less ▲]

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See detailATMOS/ATLAS-3 measurements of stratospheric chlorine and reactive nitrogen partitioning inside and outside the November 1994 Antarctic vortex
Rinsland, Curtis P.; Gunson, Michael R.; Salawitch, R. J. et al

in Geophysical Research Letters (1996), 23(17), 2365-2368

Partitioning between HCl and ClONO2 and among the main components of the reactive nitrogen family (NO, NO2, HNO3, ClONO2, N2O5, and HO2NO2) has been studied inside and outside the Antarctic stratospheric ... [more ▼]

Partitioning between HCl and ClONO2 and among the main components of the reactive nitrogen family (NO, NO2, HNO3, ClONO2, N2O5, and HO2NO2) has been studied inside and outside the Antarctic stratospheric vortex based on ATMOS profiles measured at sunrise during the 3-12 November 1994 ATLAS-3 Shuttle mission. Elevated mixing ratios of HCl in the lower stratosphere with a peak of similar to 2.9 ppbv (10(-9) parts per volume) were measured inside the vortex near 500 K potential temperature (similar to 19 km). Maximum ClONO2 mixing ratios of similar to 1.2, similar to 1.4, and similar to 0.9 ppbv near 700 K (similar to 25 km) were measured inside, at the edge, and outside the vortex, respectively. Model calculations reproduce the higher levels of HCl and NOx (NO + NO2) inside the lower stratospheric vortex both driven by photochemical processes initiated by low O3. The high HCl at low O3 results from chemical production of HCl via the reaction of enhanced Cl with CH4, limited production of ClONO2, and the descent of inorganic chlorine from higher altitudes. [less ▲]

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See detailIncrease of stratospheric carbon tetrafluoride (CF4) based on ATMOS observations from space
Zander, Rodolphe ULg; Solomon, S.; Mahieu, Emmanuel ULg et al

in Geophysical Research Letters (1996), 23(17), 2353-2356

Stratospheric volume mixing ratio profiles of carbon tetrafluoride, CF4, obtained with the Atmospheric Trace Molecule Spectroscopy (ATMOS) instrument during the ATLAS (Atmospheric Laboratory for ... [more ▼]

Stratospheric volume mixing ratio profiles of carbon tetrafluoride, CF4, obtained with the Atmospheric Trace Molecule Spectroscopy (ATMOS) instrument during the ATLAS (Atmospheric Laboratory for Applications and Science) -3 mission of 1994 are reported. Overall the profiles are nearly constant over the altitude range 20 to 50 km, indicative of the very long lifetime of CF4 in the atmosphere. In comparison to the stratospheric values of CF4 inferred from the ATMOS/Spacelab 3 mission of 1985, the 1994 concentrations are consistent with an exponential increase of (1.6 +/- 0.6)%/yr. This increase is discussed with regard to previous results and likely sources of CF4 at the ground. Further, it is shown that simultaneous measurements of N2O and CF4 provide a means of constraining the lower limit of the atmospheric lifetime of CF4 at least 2,300 years, two sigma. [less ▲]

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See detailClONO2 total vertical column abundances above the Jungfraujoch Station, 1986-1994: Long-term trend and winter-spring enhancements
Rinsland, C. P.; Zander, Rodolphe ULg; Demoulin, Philippe ULg et al

in Journal of Geophysical Research (1996), 101(D2), 3891-3899

Total vertical column abundances of chlorine nitrate (ClONO2) have been retrieved from 0.006 cm(-1) resolution solar absorption spectra recorded at the International Scientific Station of the Jungfraujoch ... [more ▼]

Total vertical column abundances of chlorine nitrate (ClONO2) have been retrieved from 0.006 cm(-1) resolution solar absorption spectra recorded at the International Scientific Station of the Jungfraujoch (ISSJ) in the Swiss Alps (altitude 3.58 km, latitude 46.5 degrees N, longitude 8.0 degrees E) on 105 days between June 1986 and November 1994. The analysis is based on spectral fittings of the ClONO2 nu(4) band Q branch at 780.21 cm(-1) and the interferences occurring in the same spectral region. The ISSJ measurements show a regular long-term increase in the ClONO2 column with an occasional factor of 2 to 3 enhancements during the midwinter to early spring. Excluding data from this time of the year, the ISSJ database reflects a linear rate of increase and la uncertainty equal to (4.0 +/- 0.7)% yr(-1) referenced to 1990.0. The corresponding ClONO2 total vertical columns for mid-1986 and mid-1994 are equal to 0.92 and 1.26 x 10(15) molecules cm(-2), respectively. The high ClONO2 columns and high HF/HCl column ratios sometimes measured during winter indicate the occasional presence of chemically processed air above the station. This is corroborated by trajectories calculated for the stratospheric air masses sounded on these occasions. [less ▲]

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See detailVertical Column Abundances of COF2 measured above the Jungfraujoch Station from ground-based infrared solar observations.
Mélen, F.; Mahieu, Emmanuel ULg; Zander, Rodolphe ULg et al

in Proceedings of Atmospheric Spectroscopy Applications (1996)

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See detailTrends of OCS, HCN, SF6, CHClF2, (HCFC-22) in the lower stratosphere from 1985 and 1994 atmospheric trace molecule spectroscopy experiment measurements near 30 degrees N latitude
Rinsland, C. P.; Mahieu, Emmanuel ULg; Zander, Rodolphe ULg et al

in Geophysical Research Letters (1996), 23(17), 2349-2352

Volume mixing ratio (VMR) profiles of OCS, HCN, SF6, and CHClF2 (HCFC-22) have been measured near 30 degrees N latitude by the Atmospheric Trace Molecule Spectroscopy Fourier transform spectrometer during ... [more ▼]

Volume mixing ratio (VMR) profiles of OCS, HCN, SF6, and CHClF2 (HCFC-22) have been measured near 30 degrees N latitude by the Atmospheric Trace Molecule Spectroscopy Fourier transform spectrometer during shuttle flights on 29 April-6 May 1985 and 3-2 November 1994. The change in the concentration of each molecule in the lower stratosphere has been derived for this 9 1/2-year period by comparing measurements between potential temperatures of 395 to 800 K (similar to 17 to 30 km altitude) relative to simultaneously measured values of the long-lived tracer N2O. Exponential rates of increase inferred for 1985-to-1994 from these comparisons are (0.1 +/- 0.4)% yr(-1) for OCS, (1.0 +/- 1.0)% yr(-1) for HCN, (8.0+/-0.7)% yr(-1) for SF6, and (8.0 +/- 1.0)% yr(-1) for CHClF2 (HCFC-22), 1 sigma. The lack of an appreciable trend for OCS suggests the background (i.e., nonvolcanic) source of stratospheric aerosol was the same during the two periods. These results are compared with trends reported in the literature. [less ▲]

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See detailThe Atmospheric Trace Molecule Spectroscopy (ATMOS) experiment: Deployment on the ATLAS Space Shuttle missions
Gunson, Michael R.; Abbas, M. M.; Abrams, M. C. et al

in Geophysical Research Letters (1996), 23(17), 2333-2336

The ATMOS Fourier transform spectrometer was flown for a fourth time on the Space Shuttle as part of the ATLAS-3 instrument payload in November 1994. More than 190 sunrise and sunset occultation events ... [more ▼]

The ATMOS Fourier transform spectrometer was flown for a fourth time on the Space Shuttle as part of the ATLAS-3 instrument payload in November 1994. More than 190 sunrise and sunset occultation events provided measurements of more than 30 atmospheric trace gases at latitudes 3-49 degrees N and 65-72 degrees S, including observations both inside and outside the Antarctic polar vortex. The instrument configuration, data retrieval methodology, and mission background are described to place in context analyses of ATMOS data presented in this issue. [less ▲]

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See detailAPRIL 1993 ARCTIC PROFILES OF STRATOSPHERIC HCL, CLONO2, AND CCL2F2 FROM ATMOSPHERIC TRACE MOLECULE SPECTROSCOPY ATLAS 2 INFRARED SOLAR OCCULTATION SPECTRA
Rinsland, C. P.; Gunson, M. R.; Abrams, M. C. et al

in Journal of Geophysical Research (1995), 100(D7), 14019-14027

Partitioning among the major components of the stratospheric odd chlorine family inside and outside of the remanent Arctic vortex has been studied on the basis of infrared solar occultation measurements ... [more ▼]

Partitioning among the major components of the stratospheric odd chlorine family inside and outside of the remanent Arctic vortex has been studied on the basis of infrared solar occultation measurements obtained by the atmospheric trace molecule spectroscopy (ATMOS) Fourier transform spectrometer during the ATLAS 2 shuttle mission (April 8-17, 1993). Profiles of hydrogen chloride (HCl) and simultaneous profiles of chlorine nitrate (ClONO2) and CFC-12 (CCl2F2) are reported for examples of in-vortex and out-of-vortex conditions. Increased ClONO2 volume-mixing ratios (VMRs) are measured in the vortex below 20 mbar (similar to 25 km altitude) with a peak ClONO2 VMR of 2.05 +/- 0.45 ppbv (10(-9) per volume) at 56 mbar (similar to 19 km altitude). The reported error correspond to la uncertainties. Simultaneous CCl2F2 and N2O measurements, combined with published empirical relations, indicate that only 0.34 +/- 0.15 ppbv, about 10% of total chlorine, was bound in organic species at the ClONO2 VMR peak in the vortex. A colocated vortex profile of HCl, referenced to simultaneous N2O VMR measurements, has been used to derive a HCl mixing ratio of 1.21 +/- 0.12 ppbv corresponding to the ClONO2 VMR peak. The internal consistency of the ATMOS measurements is demonstrated by the agreement between the total chlorine mixing ratio of 3.60 +/- 0.72 ppbv derived at the ClONO2 VMR peak in the vortex and HCl measurements of 3.37 +/- 0.37 and 3.76 +/- 0.41 ppbv at 0.56 mbar, where HCl is the only significant chlorine-bearing molecule. Outside the vortex the mixing ratio of HCl exceeds the mixing ratio of ClONO2 throughout the stratosphere. [less ▲]

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See detailVERTICAL COLUMN ABUNDANCES OF HCN DEDUCED FROM GROUND-BASED INFRARED SOLAR SPECTRA - LONG-TERM TREND AND VARIABILITY
Mahieu, Emmanuel ULg; RINSLAND, C. P.; Zander, Rodolphe ULg et al

in Journal of Atmospheric Chemistry (1995), 20(3), 299-310

A set of high-resolution IR solar spectra recorded at the International Scientific Station of the Jungfraujoch, Switzerland, from 84/06 to 93/06, and at the National Solar Observatory McMath-Pierce solar ... [more ▼]

A set of high-resolution IR solar spectra recorded at the International Scientific Station of the Jungfraujoch, Switzerland, from 84/06 to 93/06, and at the National Solar Observatory McMath-Pierce solar telescope facility on Kitt Peak, Arizona, U.S.A. from 78/05 to 92/07 have been analyzed to determine the vertical column abundances of hydrogen cyanide, HCN, above the two stations. The analysis was based on least-squares curve fitting of calculated spectra to the observations encompassing the P4 and the P8 lines of HCN respectively located at 3299.5273 and 3287.2483 cm(-1). The results obtained for the two stations indicate that no significant long-term trend affects either of the two databases; however, this analysis reveals variable increases during springtime of up to a factor of 2 in the HCN total column above the Jungfraujoch and even up to 3 above Kitt Peak. The calculated mean vertical column abundances, excluding the spring observations, are equal to (2.55 +/- 0.30) x 10(15) molec./cm(2) (S.D.) and (2.75 +/- 0.30) x 10(15) molec./cm(2) respectively above the Jungfraujoch and the Kitt Peak observatories. Based on a realistic volume mixing ratio profile, these columns translate into mean volume mixing ratios equal to 190 x 10(-12) ppv at the respective altitudes of the stations. [less ▲]

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See detailTotal ozone monitoring above the Jungfraujoch by FTIR, relative tropospheric and stratospheric contributions
Demoulin, Philippe ULg; Zander, Rodolphe ULg; Mahieu, Emmanuel ULg et al

in International conference on ozone in the lower stratosphere, Halkidiki, May 15-20, 1995 (1995)

We have attempted to discriminate between tropospheric and stratospheric burdens of ozone making up the total columns routinely derived above the Jungfraujoch from the spectral analysis of isolated lines ... [more ▼]

We have attempted to discriminate between tropospheric and stratospheric burdens of ozone making up the total columns routinely derived above the Jungfraujoch from the spectral analysis of isolated lines. For that, we have identified a number of spectral intervals containing multiple ozone transitions in which the central core of the line and the throughs between these are predominantly sensitive to, respectively, the stratospheric and lower tropospheric contents of ozone. A realistic initial volume mixing ratio profile of ozone is progressively adjusted over various layers until the root square sum of the residuals of the fit to the observations reaches a minimum. The role of the observational geometry in improving the tropospheric/stratospheric O3 ratio is also being investigated. [less ▲]

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See detailStratospheric changes monitored above the Jungfraujoch - The budgets of inorganic chlorine and fluorine since 1985.
Zander, Rodolphe ULg; Mahieu, Emmanuel ULg; Demoulin, Philippe ULg et al

in Proceedings of the 3d International Symposium on Polar Stratospheric Ozone Research (1995)

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See detailINCREASE IN LEVELS OF STRATOSPHERIC CHLORINE AND FLUORINE LOADING BETWEEN 1985 AND 1992
Gunson, M. R.; Abrams, M. C.; Lowes, L. L. et al

in Geophysical Research Letters (1994), 21(20), 2223-2226

Mixing ratios of 3.44 ppbv (parts per billion by volume) and 1.23 ppbv for HCl and HF above 50 km, surrogates for total chlorine and fluorine, have been measured by the Atmospheric Trace Molecule ... [more ▼]

Mixing ratios of 3.44 ppbv (parts per billion by volume) and 1.23 ppbv for HCl and HF above 50 km, surrogates for total chlorine and fluorine, have been measured by the Atmospheric Trace Molecule Spectroscopy (ATMOS) experiment on a March 1992 flight of the Space Shuttle. Compared to the measured values obtained on a 1985 flight, these correspond to a 37% and 62% increase for HCl and HF, respectively. The derived trend in HCl (similar to 0.13 ppbv per year) is in good agreement with the model-predicted increase in chlorine loading of 0.13 ppbv per year [Prather and Watson. 1990], and with the measured trends in HCl total column abundance from reported ground-based observations. The main source of this change can be attributed to the release of man-made chlorofluorocarbons (CFCs) and hydrochlorofluorocarbons (HCFCs). This new value for HCl represents an upper limit to the inorganic chlorine concentration in the stratosphere available for participation in photochemical processes which destroy ozone. [less ▲]

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