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See detailThe NOy budget above Jungfraujoch: long-term evolution, family partition and model comparison
Demoulin, Philippe ULg; Mahieu, Emmanuel ULg; Zander, Rodolphe ULg et al

in Abstracts presented at the NDSC 2001 Symposium: Celebrating 10 years of atmospheric research (2001)

Based on high-resolution solar spectra recorded with FTIR instruments at the University of Liège laboratory located at the Jungfraujoch NDSC station (Swiss Alps, 46.5ºN, 8ºE, altitude 3580 m), the most ... [more ▼]

Based on high-resolution solar spectra recorded with FTIR instruments at the University of Liège laboratory located at the Jungfraujoch NDSC station (Swiss Alps, 46.5ºN, 8ºE, altitude 3580 m), the most important constituents making up the NOy family have been measured consistently since the mid-1980s. They include HNO3, NO, NO2 and ClONO2, which are analyzed in terms of their vertical column abundances above the site. Related trends have been determined and assessed statistically. Among these, only ClONO2 and NO2 reveal significant long-term trends. The combined column evaluation of NOy indicates a rate of change equal to (0.1+/-0.2) %/year, thus statistically undefined and barely consistent with the evolution of the source gas N2O. Trends derived from the observations will be compared critically with those deduced from a long-term run of a 2-D stratospheric model developed at the University of Oslo. The model includes full gaseous chemistry, PSCs and sulfate particles, which vary from year to year. Comparisons with similar data found in the literature are also discussed. [less ▲]

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See detailEnhanced tropospheric HCN columns above Kitt Peak during the 1982-1983 and 1997-1998 El Nino warm phases
Rinsland, Curtis P.; Goldman, Aaron; Zander, Rodolphe ULg et al

in Journal of Quantitative Spectroscopy & Radiative Transfer (2001), 69(1), 3-8

Free tropospheric HCN columns have been derived from infrared solar spectra recorded with the National Solar Observatory Fourier transform spectrometer on Kitt Peak, Arizona (31.9ºN latitude, 111.6ºW ... [more ▼]

Free tropospheric HCN columns have been derived from infrared solar spectra recorded with the National Solar Observatory Fourier transform spectrometer on Kitt Peak, Arizona (31.9ºN latitude, 111.6ºW longitude, 2.09 km altitude) between May 1978 and May 2000. The time series show up to a factor of 2.4 enhancement during the strong El Ninos of 1982-1983 and 1997-1998, the most intense since 1970. The observations provide confirmation that HCN is a sensitive tracer of biomass burning emissions transported to the free troposphere. No statistically significant long-term trend in the HCN-free tropospheric column has been detected over the 22-year measurement period. The results illustrate the importance of long-term spectroscopic measurements for quantifying climate and atmospheric chemistry-related atmospheric changes. [less ▲]

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See detailFree tropospheric CO, C2H6, and HCN above central Europe: Recent measurements from the Jungfraujoch station including the detection of elevated columns during 1998
Rinsland, C. P.; Mahieu, Emmanuel ULg; Zander, Rodolphe ULg et al

in Journal of Geophysical Research. Atmospheres (2000), 105(D19), 24235-24249

Time series of free tropospheric carbon monoxide (CO), ethane (C2H6), and hydrogen cyanide (HCN) column abundances have been derived from observations at the International Scientific Station of the ... [more ▼]

Time series of free tropospheric carbon monoxide (CO), ethane (C2H6), and hydrogen cyanide (HCN) column abundances have been derived from observations at the International Scientific Station of the Jungfraujoch (ISSJ) at 3.58-km altitude in the Swiss Alps (latitude 46.55 degreesN, 7.98 degreesE longitude). The free troposphere was assumed to extend from 3.58 to 11 km altitude, and the related columns were derived for all three molecules from high spectral resolution infrared solar spectra recorded between January 1995 and October 1999. The three molecules show distinct seasonal cycles with maxima during winter for CO and C2H6, and during spring for HCN. These seasonal changes are superimposed on interannual variations. The tropospheric columns of all three molecules were elevated during 1998. Increases were most pronounced for HCN with enhanced values throughout the year, up to a factor of 2 in January 1998 when compared to averages of the other years. The increased tropospheric columns coincide with the period of widespread wildfires during the strong El Nino warm phase of 1997-1998. The emission enhancements above ISSJ are less pronounced, and they peaked after the increases measured above Mauna Loa (19.55 degreesN, 155.6 degreesW). Tropospheric trends for CO, C2H6, and HCN of (2.40 +/- 0.49), (0.47 +/- 0.64), and (7.00 +/- 1.61)% yr(-1)(1 sigma) were derived for January 1995 to October 1999. However, if 1998 measurements are excluded from the fit, CO and HCN trends that are not statistically significant, and a statistically significant decrease in the C2H6 tropospheric column, are inferred. Comparisons of the infrared CO columns with CO in situ surface measurements suggest that the CO free tropospheric vertical Volume mixing ratio profile generally decreases with altitude throughout the year. [less ▲]

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See detailCorrelation relationships of stratospheric molecular constituents from high spectral resolution, ground-based infrared solar absorption spectra
Rinsland, C. P.; Goldman, A.; Connor, B. J. et al

in Journal of Geophysical Research. Atmospheres (2000), 105(D11), 14637-14652

Comparisons of chemically active species with chemically inert tracers are useful to quantify transport and mixing and assess the accuracy of model predictions. We report measurements of chemically active ... [more ▼]

Comparisons of chemically active species with chemically inert tracers are useful to quantify transport and mixing and assess the accuracy of model predictions. We report measurements of chemically active species and chemically inert tracers in the stratosphere derived from the analysis of infrared solar absorption spectra recorded with a ground-based Fourier transform spectrometer operated typically at 0.005- to 0.01-cm(-1) spectral resolution. The measurements were recorded from Kitt Peak in southern Arizona (latitude 31.9 degrees N, 111.6 degrees W, 2.09 km altitude). Time series of N2O, CH4, O3, and HNO3 vertical profiles have been retrieved from measurements in microwindows. From these results, correlations between N2O and CH4 stratospheric mixing ratios and between O3 and HNO3 lower stratospheric mixing ratios have been derived. The measured correlations between N2O versus CH4 mixing ratios are compact and show little variability with respect to season in quantitative agreement with Atmospheric Trace Molecule Spectroscopy Experiment (ATMOS) spring and autumn measurements recorded near the same latitude. Lower stratospheric O3 versus HNO3 mixing ratios measured during low to moderate aerosol loading time periods also show a compact relations though the HNO3/O3 slope is a factor of 2 lower than obtained from November 1994 ATMOS measurements near the Same latitude. We also compare Kitt Peak and ATMOS N2O versus CH4 and O3 versus HNO3 relations obtained by averaging the measurements over two broad stratospheric layers. This comparison avoids bias from the a priori profiles and the limited vertical resolution of the ground-based observations. [less ▲]

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See detailStratospheric CO at tropical and mid-latitudes: ATMOS measurements and photochemical steady-state model calculations
Rinsland, C. P.; Salawitch, R. J.; Osterman, G. B. et al

in Geophysical Research Letters (2000), 27(9), 1395-1398

We characterize the spring and fall stratospheric distribution of CO at 49 degrees N-55 degrees S latitude from ATMOS profiles measured during 4 shuttle flights, Measured mixing ratios increase with ... [more ▼]

We characterize the spring and fall stratospheric distribution of CO at 49 degrees N-55 degrees S latitude from ATMOS profiles measured during 4 shuttle flights, Measured mixing ratios increase with potential temperature (theta) from 12 ppbv (10(-9) per unit volume) at 525 K, to 30-40 ppbv at 1750 K with only minor variations with latitude and season at a theta level. Evidence for some confinement near 1150 K in the developing November 1994 vortex is indicated from comparison of CO and N2O horizontal gradients. Measured CO mixing ratios at the tropical tropopause are a factor of 10 higher than values calculated with a steady-state model using standard photochemistry constrained by correlative temperatures and pressures, and ATMOS measurements including CH4 as inputs, Differences decrease with latitude at constant theta and are <20% at 800 K and all latitudes, where the CO photochemical lifetime is 40-50 days. [less ▲]

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See detailMonitoring the stratospheric chlorine budget during the past decades: the Montreal Protocol at work
Mahieu, Emmanuel ULg; Zander, Rodolphe ULg; Mélen, Francine et al

in NASDA (Ed.) Proceedings of the Quadriennal ozone symposium - Sapporo 2000 (2000)

The study of series of ground-based solar observations performed within the frame of the NDSC indicates that the rate of increase of the atmospheric loading of inorganic chlorine has progressively slowed ... [more ▼]

The study of series of ground-based solar observations performed within the frame of the NDSC indicates that the rate of increase of the atmospheric loading of inorganic chlorine has progressively slowed down, then stabilized around 1996-97, with a subsequent tendency towards a decrease. The investigation is based on total column abundances of HCl and ClONO2 measured at the Jungfraujoch station in the Swiss Alps and on stratospheric columns of HCl derived from observations at Kitt Peak National Observatory (Arizona, USA). The observed changes are compared with near-global observations of HCl around the stratopause by HALOE and with a global, best-case emission scenario of Cl-bearing ground-level source gases compiled by UNEP [less ▲]

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See detailFifteen years-trend characteristics of key stratospheric constituents monitored by FTIR above the Jungfraujoch.
Mahieu, Emmanuel ULg; Zander, Rodolphe ULg; Demoulin, Philippe ULg et al

in Harris, N. R. P.; Guirlet, M.; Amanatidis, G. T. (Eds.) Air Pollution Report 73 EUR 19340 (2000)

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See detailLong-term evolution of the loading of CH4, N2O, CO, CCl2F2, CHClF2 and SF6 above Central Europe during the last 15 years
Zander, Rodolphe ULg; Mahieu, Emmanuel ULg; Demoulin, Philippe ULg et al

in J. van Ham (Ed.) Non-CO2 greenhouse gases: scientific understanding, control and implementation (2000)

Long-term monitoring activities of some 20 atmospheric constituents are continuing at the International Scientific Station of the Jungfraujoch, Switzerland, based on remote infra-red solar observations ... [more ▼]

Long-term monitoring activities of some 20 atmospheric constituents are continuing at the International Scientific Station of the Jungfraujoch, Switzerland, based on remote infra-red solar observations with high spectral resolution Fourier transform spectrometers. As a contribution to non-CO2 greenhouse gas investigations, we report the trends observed in the vertical column abundances measured regularly since the mid-1980s for CH4, N2O, CO, CCl2F2, CHClF2 and SF6. With the exception of CO, all species show positive rates of change in their near past atmospheric loading, those of CH4, N2O and CCl2F2 having slowed significantly during the more recent years. The derived rates of change will be compared to findings resulting from ground-level in situ investigations at latitudes similar to that of the Jungfraujoch, and be interpreted in terms of resulting global loading changes. [less ▲]

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See detailTropospheric boundary layer investigations by differential ground-based solar FTIR spectrometry
Barret, Brice; Mahieu, Emmanuel ULg; Carleer, Michel et al

in Carleer, Michel; Hilton, Moira; Lamp, Thorsten (Eds.) et al Environmental Sensing and Applications (Proceedings Volume) (1999, September 16)

In order to better understand the chemistry and the transport mechanisms in the lower troposphere, a new original technique has been developed and tested. The experiment consists in recording high ... [more ▼]

In order to better understand the chemistry and the transport mechanisms in the lower troposphere, a new original technique has been developed and tested. The experiment consists in recording high resolution infrared solar absorption spectra containing signatures of important atmospheric constituents, simultaneously from the International Scientific Station of the Jungfraujoch in Switzerland [ISSJ, 3580 m a.s.l., 46.5 degrees N, 8 degrees E, Bruker 120 HR Fourier transform spectrometer (FTS)] and from a nearby valley (Grindelwald, 1070 m a.s.l., Bruker 120 M FTS). Analysis of individual spectra allows to determine vertical column abundances: differences between measurements at ISSJ and at Grindelwald enable us to retrieve the constituents' concentrations between 1070 m and 3580 m, assuming a constant volume mixing ratio in this layer. A first measurement campaign has been organized during the months of May and June 1998. After an initial period of instrument intercomparison at ISSJ, the mobile instrument was moved down in the valley and installed for one month in Grindelwald. When operated side by side at the Jungfraujoch, measurements made by both instruments showed a very good agreement (maximum bias of 1.5%). Analysis of spectra recorded synchronously at the Jungfraujoch and at Grindelwald gave average boundary layer concentrations for a selected set of tropospheric molecules, i.e. methane, nitrous oxide, carbon monoxide and ethane. Comparison with other results and with carbon monoxide in-situ measurements made at ISSJ showed a good agreement. [less ▲]

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See detailLong-lived organic compounds (Chapter 1)
Prinn, R.; Zander, Rodolphe ULg; Cunnold, D. M. et al

in Albritton; Aucamp, Pieter J.; Mégie, Gérard (Eds.) et al Scientific Assessment of Ozone Depletion: 1998 (1999)

This assessment report is a summary of the scientific community's current understanding of the stratospheric ozone layer and its relation to humankind.

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See detailPolar stratospheric descent of NOy and CO and Arctic denitrification during winter 1992-1993
Rinsland, C. P.; Salawitch, R. J.; Gunson, M. R. et al

in Journal Of Geophysical Research. Atmospheres (1999), 104(D1), 1847-1861

Observations inside the November 1994 Antarctic stratospheric vortex and inside the April 1993 remnant Arctic stratospheric vortex by the Atmospheric Trace Molecule Spectroscopy (ATMOS) Fourier transform ... [more ▼]

Observations inside the November 1994 Antarctic stratospheric vortex and inside the April 1993 remnant Arctic stratospheric vortex by the Atmospheric Trace Molecule Spectroscopy (ATMOS) Fourier transform spectrometer are reported. In both instances, elevated volume mixing ratios (VMRs) of carbon monoxide (CO) were measured. A peak Antarctic CO VMR of 60 ppbv (where 1 ppbv = 10(-9) per unit volume) was measured at a potential temperature (Theta) of 710 K (similar to 27 km), about 1 km below the altitude of a pocket of elevated NOy (total reactive nitrogen) at a deep minimum in N2O (<5 ppbv). The Arctic observations also show a region of elevated vortex CO with a peak VMR of 90 ppbv at 630-670 K (similar to 25 km) but no corresponding enhancement in NOy, perhaps because of stronger dynamical activity in the northern hemisphere polar winter and/or interannual variability in the production of mesospheric NO. By comparing vortex and extravortex observations of NOy obtained at the same N2O VMR, Arctic vortex denitrification of 5 +/- 2 ppbv at 470 K (similar to 18 km) is inferred. We show that our conclusion of substantial Arctic winter 1992-1993 denitrification is robust by comparing our extravortex observations with previous polar measurements obtained over a wide range of winter conditions. Correlations of NOy with N2O measured at the same Theta by ATMOS in the Arctic vortex and at midlatitudes on board the ER-2 aircraft several weeks later lie along the same mixing line. The result demonstrates the consistency of the two data sets and confirms that the ER-2 sampled fragments of the denitrified Arctic vortex following its breakup, An analysis of the ATMOS Arctic measurements of total hydrogen shows no evidence for significant dehydration inside the vortex. [less ▲]

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See detailVertical column abundances of COF2 above the Jungfraujoch Station: update and consolidation of the database with measurements in the nu4 band region.
Mélen, Francine; Mahieu, Emmanuel ULg; Demoulin, Philippe ULg et al

in Atmospheric Spectroscopy Applications 1999 - Proceedings (1999)

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See detailColumn Abundance measurements of formaldehyde above the Jungfraujoch.
Demoulin, Philippe ULg; Zander, Rodolphe ULg; Mélen, F. et al

in Atmospheric Spectroscopy Applications 1999 - Proceedings (1999)

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See detailQuantitative evaluation of the post-Mount Pinatubo NO2 reduction and recovery, based on 10 years of Fourier transform infrared and UV-visible spectroscopic measurements at Jungfraujoch
De Mazière, Martine; Van Roozendael, Michel; Hermans, Christian et al

in Journal of Geophysical Research (1998), 103(D9), 10849-10858

The colocation of two technically different instruments for ground-based remote sensing of NO2 total column amounts at the primary Network for the Detection of Stratospheric Change Alpine station of the ... [more ▼]

The colocation of two technically different instruments for ground-based remote sensing of NO2 total column amounts at the primary Network for the Detection of Stratospheric Change Alpine station of the Jungfraujoch (46.5°N, 8.0°E) has been exploited for mutual validation of the long-term NO2 time series from both instruments and for a quantitative evaluation of the impact of the Mount Pinatubo eruption on the NO2 abundance above this northern mid-latitude observatory. The two techniques are high-resolution Fourier transform infrared solar absorption spectrometry and zenith-sky differential optical absorption spectroscopy in the UV visible. The diurnal variation of NO2 has been simulated by a simple photochemical model that allows a comparison between the data from the two techniques. This model is shown to reproduce the observed morning to evening ratios to 2.3%, on average, which is fully adequate for the needs of this study. From the 1985–1996 combined time series of NO2 morning and evening abundances, it has been concluded that the enhanced aerosol load injected into the stratosphere by Mount Pinatubo caused a maximum NO2 reduction above the Jungfraujoch by 45% in early January 1992 that died out quasi-exponentially to zero by the beginning of 1995. [less ▲]

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See detailCorrelations of stratospheric abundances of NOy, O3, N2O, and CH4 derived from ATMOS measurements
Michelsen, H. A.; Manney, G. L.; Gunson, M. R. et al

in Journal of Geophysical Research. Atmospheres (1998), 103(D21), 28347--28359

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See detailCorrelations of stratospheric abundances of CH4 and N2O derived from ATMOS measurements
Michelsen, H. A.; Manney, G. L.; Gunson, M. R. et al

in Geophysical Research Letters (1998), 25(15), 2777--2780

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See detailRecent Characteristic Budgets of Inorganic Chlorine and Fluorine above the Jungfraujoch Station
Mahieu, Emmanuel ULg; Zander, Rodolphe ULg; Mélen, Francine et al

in Harris, N. R. P.; Kilbane-Dawe, I.; Amanatidis, G.T. (Eds.) Proceedings of the 4th European Symposium on Polar Stratospheric Ozone 1997 (1998)

Within the frame of NDSC (Network for the Detection of Stratospheric Change)-related monitoring activities conducted at the International Scientific Station of the Jungfraujoch (Swiss Alps, 46.5°N, 8.0°E ... [more ▼]

Within the frame of NDSC (Network for the Detection of Stratospheric Change)-related monitoring activities conducted at the International Scientific Station of the Jungfraujoch (Swiss Alps, 46.5°N, 8.0°E, 3580 m a.s.l.), long-term investigations of the inorganic chlorine and fluorine budgets have been pursued during the last years. They are based on the analysis of high-resolution infrared solar spectra, recorded with grating and Fourier transform state-of-the-art spectrometers. Nonlinear least squares fittings of synthetic spectra to the observations are performed over selected intervals, encompassing characteristic absorptions of HCl, ClONO2, HF and COF2; this allows the retrieval of their total vertical column abundances above the Jungfraujoch and the evaluation of their budgets. [less ▲]

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See detailGround-based FTIR Measurements from a Series of European sites during the Winter of 1995/96 and a Comparison with a 3D Chemical Transport Model: Evidence of Chlorine Activation and Ozone depletion
Paton Walsh, C.; Bell, W.; Blumenstock, T. et al

in Harris, N. R. P.; Kilbane-Dawe, I.; Amanatidis, G.T. (Eds.) Polar stratospheric ozone 1997 (1998)

Fourier transform infra-red (FTIR) measurements of stratospheric trace species have been made at a network of five ground-based sites from 79°N to 47°N during the Northern hemisphere winter of 1995/1996 ... [more ▼]

Fourier transform infra-red (FTIR) measurements of stratospheric trace species have been made at a network of five ground-based sites from 79°N to 47°N during the Northern hemisphere winter of 1995/1996. This winter was extremely cold with temperatures below the threshold for type 1 polar stratospheric cloud (PSC) formation from mid December 1995 until early March 1996 when there was a rapid warming of the stratosphere. Over 25 days experienced temperatures low enough for ice cloud (PSC type 2) formation. Vertical columns values for HCl, ClONO2, HF and HNO3 have been derived from FTIR measurements at the following sites: Ny Alesund, Spitzbergen (79°N, 12°E); Kiruna, Sweden (67°N, 21°E); Harestua, Norway (60°N, 11°E); London, England (51°N, 0°E) and the Jungfraujoch, Switzerland (48°N, 8°E), with measurements of other stratospheric trace gases, including O3 and ClO available from some of the sites. All of these sites are equipped with high resolution Bruker 120HR or 120M spectrometers, recording atmospheric spectra in the mid infrared using the Sun as a source. These measurements have been used to provide both evidence of substantial activation within large areas of the polar vortex and a subsequent O3 depletion. The measurements suggest a well mixed central vortex area surrounded by a vortex edge that may be highly variable in composition. The measurements also provide evidence of substantial mixing of activated air from the edge of the polar vortex into middle latitudes. Comparison with the SLIMCAT 3D chemical transport model highlights the underestimation of ClONO2 concentrations in the model, with subsequent implications for underestimating O3 loss. [less ▲]

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