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See detailOur Changing Atmosphere: Evidence Based on Long-Term Infrared Solar Observations at the Jungfraujoch since 1950
Zander, Rodolphe ULg; Mahieu, Emmanuel ULg; Demoulin, Philippe ULg et al

in Science of the Total Environment (2008), 391(2-3), 184-95

The Institute of Astrophysics of the University of Liege has been present at the High Altitude Research Station Jungfraujoch, Switzerland, since the late 1940s, to perform spectrometric solar observations ... [more ▼]

The Institute of Astrophysics of the University of Liege has been present at the High Altitude Research Station Jungfraujoch, Switzerland, since the late 1940s, to perform spectrometric solar observations under dry and weakly polluted high-mountain conditions. Several solar atlases of photometric quality, extending altogether from the near-ultra-violet to the middle-infrared, were produced between 1956 and 1994, first with grating spectrometers then with Fourier transform instruments. During the early 1970s, scientific concerns emerged about atmospheric composition changes likely to set in as a consequence of the growing usage of nitrogen-containing agricultural fertilisers and the industrial production of chlorine-bearing compounds such as the chlorofluorocarbons and hydro-chlorofluorocarbons. Resulting releases to the atmosphere with ensuing photolysis in the stratosphere and catalytic depletion of the protective ozone layer prompted a worldwide consortium of chemical manufacturing companies to solicit the Liege group to help in clarifying these concerns by undertaking specific observations with its existing Jungfraujoch instrumentation. The following pages evoke the main steps that led from quasi full sun-oriented studies to priority investigations of the Earth's atmosphere, in support of both the Montreal and the Kyoto Protocols. [less ▲]

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See detailSpectroscopic detection of COClF in the tropical and mid-latitude lower stratosphere
Rinsland, Curtis P.; Nassar, Ray; Boone, Christopher D. et al

in Journal of Quantitative Spectroscopy & Radiative Transfer (2007), 105(3), 467-475

We report retrievals of COClF (carbonyl chlorofluoride) based on atmospheric chemistry experiment (ACE) solar occultation spectra recorded at tropical and mid-latitudes during 2004-2005. The COClF ... [more ▼]

We report retrievals of COClF (carbonyl chlorofluoride) based on atmospheric chemistry experiment (ACE) solar occultation spectra recorded at tropical and mid-latitudes during 2004-2005. The COClF molecule is a temporary reservoir of both chlorine and fluorine and has not been measured previously by remote sensing. A maximum COClF mixing ratio of 99.7 +/- 48.0 pptv (10(-12) per unit volume, 1 sigma) is measured at 28 km for tropical and subtropical occultations (latitudes below 20 degrees in both hemispheres) with lower mixing ratios at both higher and lower altitudes. Northern hemisphere mid-latitude mixing ratios (30-50 degrees N) resulted in an average profile with a peak mixing ratio of 51.7 +/- 132.1 pptv, 1 sigma, at 27 km, also decreasing above and below that altitude. We compare the measured average profiles with the one reported set of in situ lower stratospheric mid-latitude measurements from 1986 and 1987, a previous two-dimensional (2-D) model calculation for 1987 and 1993, and a 2-D-model prediction for 2004. The measured average tropical profile is in close agreement with the model prediction; the northern mid-latitude profile is also consistent, although the peak in the measured profile occurs at a higher altitude (2.5-4.5 km offset) than in the model prediction. Seasonal average 2-D-model predictions of the COClF stratospheric distribution for 2004 are also reported. (c) 2006 Elsevier Ltd. All rights reserved. [less ▲]

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See detailRecent evolution of stratospheric inorganic chlorine (Cly) inferred from long-term ground-based FTIR observations of HCl and ClONO2
Mahieu, Emmanuel ULg; Duchatelet, Pierre ULg; Zander, Rodolphe ULg et al

in Geophysical Research Abstracts (2007, May 02), 9

Over the past decades, the increase of the stratospheric inorganic chlorine (Cly) loading has been the major cause for the ozone layer depletion, a matter of particular concern because of its ... [more ▼]

Over the past decades, the increase of the stratospheric inorganic chlorine (Cly) loading has been the major cause for the ozone layer depletion, a matter of particular concern because of its anthropogenic nature. Fortunately, appropriate decisions have been defined and put into force at the international level, leading to regulations adopted within the frame of the Montreal Protocol and its Amendments and Adjustments, and aiming at the suppression of all chlorine-bearing source gas emissions. Since its formalization, the NDSC (Network for Detection of Stratospheric Change, recently renamed NDACC, Network for the Detection of Atmospheric Composition Change) has given high priority to the monitoring of Cly based on solar observations with Fourier transform infrared (FTIR) spectrometers operated at the ground. Within this context, high-resolution solar absorption spectra recorded at Northern and Southern mid-latitudes have been analyzed to retrieve total vertical column abundances of the two main inorganic chlorine species, i.e. HCl and ClONO2. At these latitudes and in the absence of chlorine activation, these two reservoirs account for more than 92% of the total Cly loading. In this contribution, column abundance time series of HCl and ClONO2 for both the Jungfraujoch (46.5°N) and Lauder (45°S) NDACC primary stations will be presented. Comparison of these measurements with the 3-D CTM KASIMA model predictions will be shown and discussed critically, with some focus on the time period following the peak loading. Related trends will be determined and compared to expectations deduced from the most recent emission scenarios. [less ▲]

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See detailValidation of MIPAS ClONO2 measurements
Hopfner, Michael; von Clarmann, Thomas; Fischer, H. et al

in Atmospheric Chemistry and Physics (2007), 7

Altitude profiles of ClONO2 retrieved with the IMK (Institut fur Meteorologie und Klimaforschung) science-oriented data processor from MIPAS/Envisat (Michelson Interferometer for Passive Atmospheric ... [more ▼]

Altitude profiles of ClONO2 retrieved with the IMK (Institut fur Meteorologie und Klimaforschung) science-oriented data processor from MIPAS/Envisat (Michelson Interferometer for Passive Atmospheric Sounding on Envisat) mid-infrared limb emission measurements between July 2002 and March 2004 have been validated by comparison with balloon-borne (Mark IV, FIRS2, MIPAS-B), airborne (MIPAS-STR), ground-based (Spitsbergen, Thule, Kiruna, Harestua, Jungfraujoch, Izana, Wollongong, Lauder), and spaceborne (ACE-FTS) observations. With few exceptions we found very good agreement between these instruments and MIPAS with no evidence for any bias in most cases and altitude regions. For balloon-borne measurements typical absolute mean differences are below 0.05 ppbv over the whole altitude range from 10 to 39 km. In case of ACE-FTS observations mean differences are below 0.03 ppbv for observations below 26 km. Above this altitude the comparison with ACE-FTS is affected by the photochemically induced diurnal variation of ClONO2. Correction for this by use of a chemical transport model led to an overcompensation of the photochemical effect by up to 0.1 ppbv at altitudes of 30-35 km in case of MIPAS-ACE-FTS comparisons while for the balloon-borne observations no such inconsistency has been detected. The comparison of MIPAS derived total column amounts with ground-based observations revealed no significant bias in the MIPAS data. Mean differences between MIPAS and FTIR column abundances are 0.11 +/- 0.12 x 10(14) cm(-2) (1.0 +/- 1.1%) and -0.09 +/- 0.19 x 10(14) cm(-2) (-0.8 +/- 1.7%), depending on the coincidence criterion applied. chi(2) tests have been performed to assess the combined precision estimates of MIPAS and the related instruments. When no exact coincidences were available as in case of MIPAS-FTIR or MIPAS-ACE-FTS comparisons it has been necessary to take into consideration a coincidence error term to account for chi(2) deviations. From the resulting chi(2) profiles there is no evidence for a systematic over/underestimation of the MIPAS random error analysis. [less ▲]

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See detailFTIR Observations at the Jungfraujoch Station for long-term monitoring of the Troposphere and Validation of the Space-based Sensors.
Mahieu, Emmanuel ULg; Zander, Rodolphe ULg; Demoulin, Philippe ULg et al

in Burrows, J.; Borrell, P. (Eds.) Measuring Tropospheric Trace Constituents from Space. (2007)

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See detailOptimisation of retrieval strategies using Jungfraujoch high-resolution FTIR observations for long-term trend studies and satellite validation.
Mahieu, Emmanuel ULg; Servais, Christian ULg; Duchatelet, Pierre ULg et al

in Burrows, J.; Borrell, P. (Eds.) Observing Tropospheric Trace Constituents from Space. (2007)

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See detailFirst space-based observations of formic acid (HCOOH): Atmospheric Chemistry Experiment austral spring 2004 and 2005 Southern Hemisphere tropical-mid-latitude upper tropospheric measurements
Rinsland, Curtis P.; Boone, Christopher D.; Bernath, Peter F. et al

in Geophysical Research Letters (2006), 33(23),

The first space-based measurements of upper tropospheric ( 110 - 300 hPa) formic acid (HCOOH) are reported from 0.02 cm(-1) resolution Atmospheric Chemistry Experiment (ACE) Fourier transform spectrometer ... [more ▼]

The first space-based measurements of upper tropospheric ( 110 - 300 hPa) formic acid (HCOOH) are reported from 0.02 cm(-1) resolution Atmospheric Chemistry Experiment (ACE) Fourier transform spectrometer solar occultation measurements at 16 degrees S - 43 degrees S latitude during late September to early October in 2004 and 2005. A maximum upper tropospheric HCOOH mixing ratio of 3.13 +/- 0.02 ppbv ( 1 ppbv = 10(-9) per unit volume), 1 sigma, at 10.5 km altitude was measured during 2004 at 29.97 degrees S latitude and a lower maximum HCOOH mixing ratio of 2.03 +/- 0.28 ppbv, at 9.5 km altitude was measured during 2005. Fire counts, back trajectories, and correlations of HCOOH mixing ratios with ACE simultaneous measurements of other fire products confirm the elevated HCOOH mixing ratios originated primarily from tropical fire emissions. A HCOOH emission factor relative to CO of 1.99 +/- 1.34 g kg(-1) during 2004 in upper tropospheric plumes is inferred from a comparison with lower mixing ratios measured during the same time period assuming HITRAN 2004 spectroscopic parameters. [less ▲]

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See detailA global inventory of stratospheric chlorine in 2004
Nassar, Ray; Bernath, Peter; Boone, Christopher D. et al

in Journal of Geophysical Research. Atmospheres (2006), 111(D22), 22312

[1] Total chlorine (Cl-TOT) in the stratosphere has been determined using the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) measurements of HCl, ClONO2, CH3Cl, CCl4, CCl3F (CFC ... [more ▼]

[1] Total chlorine (Cl-TOT) in the stratosphere has been determined using the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) measurements of HCl, ClONO2, CH3Cl, CCl4, CCl3F (CFC-11), CCl2F2 (CFC-12), CHClF2 (HCFC-22), CCl2FCClF2 (CFC-113), CH3CClF2 (HCFC-142b), COClF, and ClO supplemented by data from several other sources, including both measurements and models. Separate chlorine inventories were carried out in five latitude zones (60 degrees - 82 degrees N, 30 degrees - 60 degrees N, 30 degrees S - 30 degrees N, 30 degrees - 60 degrees S, and 60 degrees - 82 degrees S), averaging the period of February 2004 to January 2005 inclusive, when possible, to deal with seasonal variations. The effect of diurnal variation was avoided by only using measurements taken at local sunset. Mean stratospheric Cl-TOT values of 3.65 ppbv were determined for both the northern and southern midlatitudes (with an estimated 1 sigma accuracy of +/- 0.13 ppbv and a precision of +/- 0.09 ppbv), accompanied by a slightly lower value in the tropics and slightly higher values at high latitudes. Stratospheric Cl-TOT profiles in all five latitude zones are nearly linear with a slight positive slope in ppbv/km. Both the observed slopes and pattern of latitudinal variation can be interpreted as evidence of the beginning of a decline in global stratospheric chlorine, which is qualitatively consistent with the mean stratospheric circulation pattern and time lag necessary for transport. [less ▲]

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See detailLong-term trend of CH4 at northern mid-latitudes: Comparison between ground-based infrared solar and surface sampling measurements
Rinsland, Curtis P.; Goldman, Aaron; Elkins, James W. et al

in Journal of Quantitative Spectroscopy & Radiative Transfer (2006), 97(3), 457-466

We report average tropospheric CH4 volume mixing ratios retrieved from a 27 year time series of high spectral resolution infrared solar absorption measurements recorded between May 1977 and July 2004 at ... [more ▼]

We report average tropospheric CH4 volume mixing ratios retrieved from a 27 year time series of high spectral resolution infrared solar absorption measurements recorded between May 1977 and July 2004 at the US National Solar Observatory station on Kitt Peak (31.9 degrees N, 111.6 degrees W, 2.09 km altitude) and their comparison with surface in situ sampling measurements recorded between 1983 and 2004 at the Climate Monitoring and Diagnostics Laboratory (CMDL) station at Niwot Ridge, Colorado (40.0 degrees N, 105.5 degrees W, 3013 m altitude). The two measurement sets therefore overlap for the 1983-2004 time period. An average tropospheric volume mixing ratios of 1814 +/- 48 ppbv (1 ppbv = 10(-9) per unit volume) has been derived from the solar absorption time series with a best-fit increase rate trend equal to 8.26 +/- 2.20 ppbv yr(-1) in 1983 decreasing to 1.94 +/- 3.69 ppbv yr(-1) in 2003. The CMDL measurements also show a continuous long-term CH4 volume mixing ratio rise, with subsequent slowing down. A mean ratio of the retrieved average tropospheric volume mixing ratio to the CMDL volume mixing ratio for the overlapping time period of 1.038 +/- 0.034 indicates agreement between both data sets within the quantified experimental errors. (C) 2005 Elsevier Ltd. All rights reserved. [less ▲]

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See detailLong-term stratospheric carbon tetrafluoride (CF4) increase inferred from 1985-2004 infrared space-based solar occultation measurements
Rinsland, Curtis P.; Mahieu, Emmanuel ULg; Zander, Rodolphe ULg et al

in Geophysical Research Letters (2006), 33(2),

The long-term stratospheric carbon tetrafluoride (CF4) increase has been determined from infrared high spectral resolution solar occultation Fourier transform spectrometer measurements between 3 and 50 ... [more ▼]

The long-term stratospheric carbon tetrafluoride (CF4) increase has been determined from infrared high spectral resolution solar occultation Fourier transform spectrometer measurements between 3 and 50 hPa (similar to 20 to 40 km altitude) and latitudes from 50 degrees N to 50 degrees S during 1985, 1992, 1993, 1994, and 2004. The 1985 to 1994 measurements were recorded from the ATMOS ( Atmospheric Trace MOlecule Spectroscopy) instrument at 0.01 cm(-1) resolution and in 2004 by the Atmospheric Chemistry Experiment ( ACE) instrument at 0.02 cm(-1) resolution. Stratospheric volume mixing ratios, inferred from a polynomial fit to averages from the time periods considered here, increased from 49.37 +/- 2.60 pptv (10(-12) per unit volume) in 1985 to 58.38 +/- 4.14 pptv in 1992, 60.46 +/- 2.97 pptv in 1993, 60.11 +/- 3.60 pptv in 1994 and to 70.45 +/- 3.40 pptv in 2004. The stratospheric CF4 mixing ratio has continued to increase but at a slower rate than in previous years, for example, (1.14 +/- 0.68)% yr(-1) in 2004 as compared to (2.77 +/- 0.47)% yr(-1) in 1985, 1 sigma. Correlations of CF4 with N2O taking into account the increase of N2O with time also show the increase in the stratospheric CF4 burden over the two decade measurement time span. Our space-based measurements show that the slowdown in the rate of CF4 accumulation previously reported from surface measurements through 1997 has propagated to the stratosphere and is continuing. Citation: Rinsland, C. P., E. Mahieu, R. Zander, R. Nassar, P. Bernath, C. Boone, and L. S. Chiou (2006), Long-term stratospheric carbon tetrafluoride (CF4) increase inferred from 1985-2004 infrared space-based solar occultation measurements, Geophys. Res. Lett., 33, L02808, doi:10.1029/2005GL024709. [less ▲]

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See detailEvolution of a dozen non-CO2 greenhouse gases above Central Europe since the mid-1980s.
Zander, Rodolphe ULg; Mahieu, Emmanuel ULg; Demoulin, Philippe ULg et al

in Proceedings of the 4th International Symposium on Non-CO2 Greenhouse Gases (2006)

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See detailTrends of HF, HCl, CCl2F2, CCl3F, CHClF2 (HCFC-22), and SF6 in the lower stratosphere from Atmospheric Chemistry Experiment (ACE) and Atmospheric Trace Molecule Spectroscopy (ATMOS) measurements near 30 degrees N latitude
Rinsland, Curtis P.; Boone, Christopher D.; Nassar, Ray et al

in Geophysical Research Letters (2005), 32(16),

[ 1] Volume mixing ratios ( VMRs) of HF, HCl, CCl2F2, CHClF2 ( HCFC-22), and SF6 in the lower stratosphere have been derived from solar occultation measurements recorded with spaceborne high resolution ... [more ▼]

[ 1] Volume mixing ratios ( VMRs) of HF, HCl, CCl2F2, CHClF2 ( HCFC-22), and SF6 in the lower stratosphere have been derived from solar occultation measurements recorded with spaceborne high resolution Fourier transform spectrometers. Atmospheric Chemistry Experiment ( ACE) VMRs measured during 2004 have been compared with those obtained in 1985 and 1994 by the Atmospheric Trace MOlecule Spectroscopy ( ATMOS) instrument. Trends are estimated by referencing the measured VMRs to those of the long-lived constituent N2O to account for variations in the dynamic history of the sampled air masses. Pressure-gridded measurements covering 10-100 hPa ( similar to 16 to 30 km altitude) were used in the analysis that includes typically 25 degrees N-35 degrees N latitude. The VMR changes provide further evidence of the impact of the emission restrictions imposed by the Montreal Protocol and its strengthening amendments and adjustments and are consistent with model predictions and known sources and sinks of halocarbons. Decreases in the lower stratospheric mixing ratios of CCl3F and HCl are measured in 2004 with respect to 1994, providing important confirmation of recent ground-based solar absorption measurements of a decline in inorganic chlorine. Trends estimates are compared with other reported measurements and model predictions. [less ▲]

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See detailComparisons between ACE-FTS and ground-based measurements of stratospheric HCl and ClONO2 loadings at northern latitudes
Mahieu, Emmanuel ULg; Zander, Rodolphe ULg; Duchatelet, Pierre ULg et al

in Geophysical Research Letters (2005), 32(15),

We report first comparisons of stratospheric column abundances of hydrogen chloride (HCl) and chlorine nitrate (ClONO2) derived from infrared solar spectra recorded in 2004 at selected northern latitudes ... [more ▼]

We report first comparisons of stratospheric column abundances of hydrogen chloride (HCl) and chlorine nitrate (ClONO2) derived from infrared solar spectra recorded in 2004 at selected northern latitudes by the spaceborne Atmospheric Chemistry Experiment-Fourier Transform Spectrometer (ACE-FTS) and by Fourier transform infrared (FTIR) instruments at the NDSC (Network for Detection of Stratospheric Change)-affiliated sites of Thule ( Greenland), Kiruna ( Sweden), Jungfraujoch ( Switzerland), and Egbert and Toronto ( Canada). Overall, and within the respective uncertainties of the independent measurement approaches, the comparisons show that the ACE-FTS measurements produce very good stratospheric volume mixing ratio profiles. Their internal precision allows to identify characteristic distribution features associated with latitudinal, dynamical, seasonal and chemical changes occurring in the atmosphere. [less ▲]

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See detailAtmospheric Chemistry Experiment (ACE): Mission overview
Bernath, Peter; McElroy, C. T.; Abrams, Mark et al

in Geophysical Research Letters (2005), 32(15),

SCISAT-1, also known as the Atmospheric Chemistry Experiment ( ACE), is a Canadian satellite mission for remote sensing of the Earth's atmosphere. It was launched into low Earth circular orbit ( altitude ... [more ▼]

SCISAT-1, also known as the Atmospheric Chemistry Experiment ( ACE), is a Canadian satellite mission for remote sensing of the Earth's atmosphere. It was launched into low Earth circular orbit ( altitude 650 km, inclination 74 degrees) on 12 Aug. 2003. The primary ACE instrument is a high spectral resolution (0.02 cm(-1)) Fourier Transform Spectrometer (FTS) operating from 2.2 to 13.3 mm ( 750 - 4400 cm(-1)). The satellite also features a dual spectrophotometer known as MAESTRO with wavelength coverage of 285 - 1030 nm and spectral resolution of 1 - 2 nm. A pair of filtered CMOS detector arrays records images of the Sun at 0.525 and 1.02 mu m. Working primarily in solar occultation, the satellite provides altitude profile information ( typically 10 - 100 km) for temperature, pressure, and the volume mixing ratios for several dozen molecules of atmospheric interest, as well as atmospheric extinction profiles over the latitudes 85 degrees N to 85 degrees S. This paper presents a mission overview and some of the first scientific results. [less ▲]

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See detailEvolution of a dozen non-CO2 greenhouse gases above central Europe since the mid-1980s
Zander, Rodolphe ULg; Mahieu, Emmanuel ULg; Demoulin, Philippe ULg et al

in Environmental Sciences (2005), 2(2-3), 295-303

High-resolution infrared solar observations have been conducted consistently since the mid-1980s at the International Scientific Station of the Jungfraujoch, Switzerland, by the GIRPAS-ULg team (Groupe ... [more ▼]

High-resolution infrared solar observations have been conducted consistently since the mid-1980s at the International Scientific Station of the Jungfraujoch, Switzerland, by the GIRPAS-ULg team (Groupe Infra-Rouge de Physique Atmosphrique et Solaire-University of Lige), and by colleagues from the Belgian Institute for Space Aeronomy and from the Royal Observatory of Belgium, Brussels. These observations were performed with state-of-the-art Fourier transform infrared (FTIR) spectrometers, revealing specific absorption features of over 20 atmospheric gases in the middle-infrared. Related spectrometric analyses have allowed the derivation of their burdens, seasonal and inter-annual variability, as well as their long-term evolution. In addition to updates of long-term changes for CCl2F2, CHClF2, CH4, N2O, SF6, CO, C2H6 and C2H2 already dealt with at previous Non-CO2 Greenhouse Gases (NCGG) symposia, this paper further reports temporal evolutions observed during the past two decades for a series of other source gases, namely OCS, HCN, CCl3F and CCl4, which also have direct or indirect effects on the radiation balance of the troposphere and on the stratospheric ozone layer. [less ▲]

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See detailSulphur hexafluoride (SF6): comparison of FTIR-measurements at three sites and determination of its trend in the northern hemisphere
Krieg, Juergen; Notholt, Justus; Mahieu, Emmanuel ULg et al

in Journal of Quantitative Spectroscopy & Radiative Transfer (2005), 92(3), 383-392

Fourier transform infrared spectrometry has been used to retrieve the total column abundances of SF6 at three locations in the northern hemisphere, i.e., the Ny- Angstromlesund site in Spitsbergen/Norway ... [more ▼]

Fourier transform infrared spectrometry has been used to retrieve the total column abundances of SF6 at three locations in the northern hemisphere, i.e., the Ny- Angstromlesund site in Spitsbergen/Norway at 79degreesN, the Jungfraujoch observatory in Switzerland at 47degreesN and the Kitt Peak observatory in Arizona, USA, at 32degreesN. The total column results have been converted to average tropospheric mixing ratios. The mean increases in these mixing ratios have been found to be, equal to 0.31 +/- 0.08 pptv yr(-1) at Ny Angstromlesund, 0.24 +/- 0.01 pptv yr(-1) at the Jungfraujoch and 0.28 +/- 0.09 pptv yr(-1) at Kitt Peak for the common period March 1993 to March 2002, in agreement with corresponding CMDL data (0.21 +/- 0.0002 pptv yr(-1)) at the surface. The limited accuracy of the Ny Angstromlesund and Kitt Peak data results from strong tropospheric water vapour interferences at these lower altitude sites. Observations at all three locations show that SF6 is Still accumulating in the atmosphere. Extrapolations of linear and second-order fits to the Jungfraujoch data predict tropospheric mixing ratios of SF6, respectively equal to 16.4 +/- 0.5 and. 14.7 +/- 0.6 in 2050, and 28.2 +/- 0.9 and 22.2 +/- 10.8 pptv in 2100, significantly, lower than those reported in the literature so far. (C) 2004 Elsevier Ltd. All, rights reserved. [less ▲]

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See detailLong-term evolution in the tropospheric concentration of chlorofluorocarbon 12 (CCl2F2) derived from high-spectral resolution infrared solar absorption spectra: retrieval and comparison with in situ surface measurements
Rinsland, Curtis P.; Goldman, Aaron; Mahieu, Emmanuel ULg et al

in Journal of Quantitative Spectroscopy & Radiative Transfer (2005), 92(2), 201-209

The average tropospheric volume mixing ratios of chlorofluorocarbon 12 (CCl2F2) have been retrieved from high-spectral resolution ground-based infrared solar-absorption spectra recorded from March 1982 to ... [more ▼]

The average tropospheric volume mixing ratios of chlorofluorocarbon 12 (CCl2F2) have been retrieved from high-spectral resolution ground-based infrared solar-absorption spectra recorded from March 1982 to October 2003 with the McMath Fourier transform spectrometer at the US National Solar Observatory facility on Kitt Peak in southern Arizona (31.9degreesN, 111.6degreesW, 2.09 km altitude). The retrievals are based on fits to the unresolved v(8) band Q-branches near 922 cm(-1) using the SFIT2 retrieval algorithm. The annual increase rate was equal to (16.88 +/- 1.37) parts per trillion (10(-12)) by volume at the beginning of the time series, March 1982, or (4.77 +/- 0.04)%, 1 sigma, declining progressively to (2.49 +/- 1.24) parts per trillion, by volume at the end, October 2003, or (0.46 +/- 0.24)%, 1 sigma. Average tropospheric mixing ratios from the solar spectra have been compared with average surface flask and in situ sampling measurements from the Climate Monitoring and Diagnostics Laboratory (CMDL) station at Niwot Ridge, CO, (USA) (40.0degreesN, 105.5degreesW, 3013 m altitude). The average ratio and standard deviation of the monthly means of the retrieved tropospheric mixing ratios relative to the CMDL surface mixing ratios is (1.01 +/- 0.03) for the overlapping time period. Both datasets demonstrate the progressive impact of the Montreal protocol and its strengthening amendments on the trend of CCl2F2, though a tropospheric decrease has yet to be observed. (C) 2004 Elsevier Ltd. All rights reserved. [less ▲]

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See detailRecent Evolution of atmospheric OCS above the Jungfraujoch station : implications for the stratospheric aerosol layer.
Mahieu, Emmanuel ULg; Zander, Rodolphe ULg; Demoulin, Philippe ULg et al

in Proceedings of the Atmospheric Spectroscopy Applications. (2005)

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See detailFree tropospheric measurements of formic acid (HCOOH) from infrared ground-based solar absorption spectra: Retrieval approach, evidence for a seasonal cycle, and comparison with model calculations
Rinsland, Curtis P.; Mahieu, Emmanuel ULg; Zander, Rodolphe ULg et al

in Journal of Geophysical Research. Atmospheres (2004), 109(D18),

The seasonal variation of the free tropospheric volume mixing ratio of formic acid (HCOOH) has been derived from high-spectral-resolution solar absorption spectra recorded with the Fourier transform ... [more ▼]

The seasonal variation of the free tropospheric volume mixing ratio of formic acid (HCOOH) has been derived from high-spectral-resolution solar absorption spectra recorded with the Fourier transform spectrometer in the U. S. National Solar Observatory facility on Kitt Peak (31.9degreesN, 111.6degreesE, 2.09 km altitude) at a typical spectral resolution of 0.005 cm(-1). The spectra have been analyzed with the SFIT2 algorithm, which is based on a semiempirical application of the optimal estimation method. Absorption by HCOOH is weak in these solar spectra, but successful retrievals have been obtained with a new procedure that fits the HCOOH nu(6) band Q branch at 1105 cm(-1) simultaneously with a window to account for a temperature-sensitive HDO line, which overlaps the HCOOH Q branch. After retaining only the best measurements from a database extending from June 1980 to October 2002 the retrievals show a seasonal variation, with a summer maximum and a winter minimum. Average 2.09-10 km volume mixing ratios binned in 3 month intervals range from a maximum of 792+/-323 parts per trillion by volume (pptv), or 10(-12), in July-September to a minimum of 313+/-175 pptv in October-December, with the uncertainties corresponding to statistical means from daily averages. The results are compared with previously reported measurements and model calculations. [less ▲]

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