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See detailThe recent increase of atmospheric methane from 10 years of ground-based NDACC FTIR observations since 2005
Bader, Whitney ULiege; Bovy, Benoît ULiege; Conway, Stephanie et al

in Atmospheric Chemistry and Physics (2017)

Changes of atmospheric methane total columns (CH4/ since 2005 have been evaluated using Fourier transform infrared (FTIR) solar observations carried out at 10 ground-based sites, affiliated to the Network ... [more ▼]

Changes of atmospheric methane total columns (CH4/ since 2005 have been evaluated using Fourier transform infrared (FTIR) solar observations carried out at 10 ground-based sites, affiliated to the Network for Detection of Atmospheric Composition Change (NDACC). From this, we find an increase of atmospheric methane total columns of 0.31±0.03 %/year (2-sigma level of uncertainty) for the 2005–2014 period. Comparisons with in situ methane measurements at both local and global scales show good 10 agreement. We used the GEOS-Chem chemical transport model tagged simulation, which accounts for the contribution of each emission source and one sink in the total methane, simulated over 2005–2012. After regridding according to NDACC vertical layering using a conservative 15 regridding scheme and smoothing by convolving with respective FTIR seasonal averaging kernels, the GEOS-Chem simulation shows an increase of atmospheric methane total columns of 0.35±0.03 %/year between 2005 and 2012, which is in agreement with NDACC measurements over the same time period (0.30±0.04 %/year, averaged over 10 stations). Analysis of the GEOS-Chem-tagged simulation allows us to quantify the contribution of each tracer to the global methane change since 2005. We find that natural sources such as wetlands and biomass burning contribute to the interannual variability of methane. However, anthropogenic emissions, such as coal mining, and gas and oil transport and exploration, which are mainly emitted in the Northern Hemisphere and act as secondary contributors to the global budget of methane, have played a major role in the increase of atmospheric methane observed since 2005. Based on the GEOS-Chem-tagged simulation, we discuss possible cause(s) for the increase of methane since 2005, which is still unexplained. [less ▲]

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See detailThe evolution of the inorganic fluorine budget since the mid-1980s based on FTIR measurements at northern mid-latitudes
Duchatelet, Pierre ULiege; Feng, Wuhu; Chipperfield, Martyn et al

in Geophysical Research Abstracts (2011)

Fluorine enters the stratosphere principally in the form of CFCs (chlorofluorocarbons, mainly CFC-12 and CFC-11), HCFCs (hydrochlorofluorocarbons, mainly HCFC-22) and HFCs (hydrofluorocarbons, mainly HFC ... [more ▼]

Fluorine enters the stratosphere principally in the form of CFCs (chlorofluorocarbons, mainly CFC-12 and CFC-11), HCFCs (hydrochlorofluorocarbons, mainly HCFC-22) and HFCs (hydrofluorocarbons, mainly HFC-134a) which have been (or are still) widely emitted at ground level by human activities. In the lower stratosphere, the photolysis of these halogenated source gases leads to the formation of the two fluorine reservoirs COClF and COF2. The subsequent photolysis of these two compounds frees F atoms, which principally react with CH4 and H2O to form the extremely stable HF gas, by far the dominant fluorine reservoir in the middle and upper stratosphere. Despite the fact that fluorine does not significantly contribute in stratospheric ozone depletion, measurements of the concentrations of individual F-containing species in different altitude ranges of the atmosphere are important as they reflect the amounts of anthropogenic gases transported into the middle atmosphere as well as their decomposition. Such measurements also provide insight into the partitioning between major fluorine source gases (which are potent greenhouse gases) and reservoirs and allows a global inventory of organic (CFy), inorganic (Fy) and total (FTOT) fluorine burdens to be monitored as a function of time. Indeed, regular updates of such inventories are important as the partitioning between F-containing gases in the stratosphere is continually evolving as emissions of anthropogenic gases from the surface change, principally as a consequence of the progressive ban on the production of CFCs and HCFCs adopted by the Montreal Protocol and its subsequent Amendments and Adjustments. To complement recent studies regarding fluorine species (Duchatelet et al., 2009, 2010, 2011; Mahieu et al., 2011), this communication presents the time series of the inorganic fluorine budget Fy over the last twenty-five years, based on HF and COF2 total column amounts derived from high resolution Fourier transform infrared (FTIR) solar spectra recorded at Jungfraujoch (46.5°N, 8.0°E, 3580m asl). A trend analysis of our HF, COF2 and Fy time series is performed and discussed in the context of past and current emissions of halogenated source gases. Comparisons with model and space data are also included. [less ▲]

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See detailUpdating hydrogen fluoride (HF) FTIR time series above Jungfraujoch: comparison of two retrieval algorithms and impact of line shape models
Duchatelet, Pierre ULiege; Demoulin, Philippe ULiege; Hase, Frank et al

Poster (2010, May)

Fluorine enters the stratosphere mainly in the form of chlorofluorocarbons (CFCs; principally CFC-11 and CFC-12) and tetrafluoromethane (CF4), which have been widely emitted at ground level by human ... [more ▼]

Fluorine enters the stratosphere mainly in the form of chlorofluorocarbons (CFCs; principally CFC-11 and CFC-12) and tetrafluoromethane (CF4), which have been widely emitted at ground level by human activities over the past few decades. In the lower stratosphere, the photolysis of the long-lived CFC-11 (CCl3F) and CFC-12 (CCl2F2), whose emissions from the ground have been progressively phased out by the Montreal Protocol and its successive Amendments and Adjustments, leads to the formation of the two reservoirs: COClF and COF2. Subsequent photolysis of these two compounds then liberates F atoms, which could quickly react with CH4, H2O or H2 to form the extreme stable hydrogen fluoride (HF) gas. The formation of HF by these reactions is significant, as they make HF the largest fluorine reservoir in the middle and upper stratosphere. Despite the fact that fluorine does not directly participate in ozone depletion, measurements of the concentration of individual F-containing species at different altitude of the atmosphere are important as they reflect the amounts of anthropogenic gases – which also often bear ozone-threatening Cl atoms - transported into the middle atmosphere as well as their decomposition. Since the first detection of hydrogen fluoride in the Earth’s atmosphere by Zander (1975), several studies dealing with HF total column amounts derived from ground-based Fourier transform infrared (FTIR) observations at several latitudes in both hemispheres have been published. In addition, these last years have seen the emergence of more sophisticated retrieval algorithms (e.g. SFIT-2, PROFFIT) allowing to inverse total or partial columns as well as vertical distribution of the target gas from ground-based FTIR spectra. In this contribution, we propose to compare HF total columns derived from FTIR high-resolution ground-based observations performed at the Jungfraujoch (46.5°N, 8.0°E, 3580 m asl) by using two different retrieval codes: SFIT-2 v.3.91 and PROFFIT v.9.5. The impact of spectroscopic parameters (Voigt line shape model versus Galatry model line shape) on HF retrievals is also analyzed. References: Zander, R.: Présence de HF dans la stratosphère supérieure, C.R. Acad. Sci. Paris. Série B., 281, 213-214, 1975. [less ▲]

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See detailHydrogen fluoride total and partial column time series above the Jungfraujoch from long-term FTIR measurements: Impact of the line-shape model, characterization of the error budget and seasonal cycle, and comparison with satellite and model data
Duchatelet, Pierre ULiege; Demoulin, Philippe ULiege; Hase, Frank et al

in Journal of Geophysical Research. Atmospheres (2010), 115

Time series of hydrogen fluoride (HF) total columns have been derived from ground-based Fourier transform infrared (FTIR) solar spectra recorded between March 1984 and December 2009 at the International ... [more ▼]

Time series of hydrogen fluoride (HF) total columns have been derived from ground-based Fourier transform infrared (FTIR) solar spectra recorded between March 1984 and December 2009 at the International Scientific Station of the Jungfraujoch (Swiss Alps, 46.5°N, 8.0°E, 3580 m asl) with two high resolution spectrometers (one home-made and one Bruker 120-HR). Solar spectra have been inverted with the PROFFIT 9.5 algorithm, using the optimal estimation method. An inter-comparison of HF total columns retrieved with PROFFIT and SFIT-2 – the other reference algorithm in the FTIR community - is performed for the first time. The effect of a Galatry line shape model on HF retrieved total columns and vertical profiles, on the residuals of the fits and on the error budget is also quantified. Information content analysis indicates that, in addition to HF total vertical abundance, three independent stratospheric HF partial columns can be derived from our Bruker spectra. A complete error budget has been established and indicates that the main source of systematic error is linked to HF spectroscopy and that the random error affecting our HF total columns does not exceed 2.5%. Ground-based middle and upper stratospheric HF amounts have been compared to satellite data collected by the HALOE or ACE-FTS instruments. Comparisons of our FTIR HF total and partial columns with runs performed by two 3D numerical models (SLIMCAT and KASIMA) are also included. Finally, FTIR and model HF total and partial columns time series have been analyzed to derive the main characteristics of their seasonal cycles. [less ▲]

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See detailAn approach to retrieve information on the carbonyl fluoride (COF2) vertical distributions above Jungfraujoch by FTIR multi-spectrum multi-window fitting
Duchatelet, Pierre ULiege; Mahieu, Emmanuel ULiege; Ruhnke, Roland et al

in Atmospheric Chemistry and Physics (2009), 9

We present an original multi-spectrum fitting procedure to retrieve volume mixing ratio (VMR) profiles of carbonyl fluoride (COF2) from ground-based high resolution Fourier transform infrared (FTIR) solar ... [more ▼]

We present an original multi-spectrum fitting procedure to retrieve volume mixing ratio (VMR) profiles of carbonyl fluoride (COF2) from ground-based high resolution Fourier transform infrared (FTIR) solar spectra. The multi-spectrum approach consists of simultaneously combining, during the retrievals, all spectra recorded consecutively during the same day and with the same resolution. Solar observations analyzed in this study with the SFIT-2 v3.91 fitting algorithm correspond to more than 2900 spectra recorded between January 2000 and December 2007 at high zenith angles, with a Fourier Transform Spectrometer operated at the high-altitude International Scientific Station of the Jungfraujoch (ISSJ, 46.5° N latitude, 8.0° E longitude, 3580 m altitude), Switzerland. The goal of the retrieval strategy described here is to provide information about the vertical distribution of carbonyl fluoride. The microwindows used are located in the ν4 or in the ν4 COF2 infrared (IR) absorption bands. Averaging kernel and eigenvector analysis indicates that our FTIR retrieval is sensitive to COF2 inversion between 17 and 30 km, with the major contribution to the retrieved information always coming from the measurement. Moreover, there was no significant bias between COF2 partial columns, total columns or VMR profiles retrieved from the two bands. For each wavenumber region, a complete error budget including all identified sources has been carefully established. In addition, comparisons of FTIR COF2 17–30 km partial columns with KASIMA and SLIMCAT 3-D CTMs are also presented. If we do not notice any significant bias between FTIR and SLIMCAT time series, KASIMA COF2 17–30 km partial columns are lower of around 25%, probably due to incorrect lower boundary conditions. For each times series, linear trend estimation for the 2000–2007 time period as well as a seasonal variation study are also performed and critically discussed. For FTIR and KASIMA time series, very low COF2 growth rates (0.4±0.2%/year and 0.3±0.2%/year, respectively) have been derived. However, the SLIMCAT data set gives a slight negative trend (−0.5±0.2%/year), probably ascribable to discontinuities in the meteorological data used by this model. We further demonstrate that all time series are able to reproduce the COF2 seasonal cycle, which main seasonal characteristics deduced from each data set agree quite well. [less ▲]

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See detailDetermination of isotopic fractionation delta13C of methane from ground-based FTIR observations performed at the Jungfraujoch
Duchatelet, Pierre ULiege; Mahieu, Emmanuel ULiege; Sussmann, Ralf et al

Poster (2009, April)

Atmospheric methane (CH4) is a strong greenhouse gas that has important chemical impacts on both the troposphere and the stratosphere. In the troposphere, oxidation of methane is a major regulator of OH ... [more ▼]

Atmospheric methane (CH4) is a strong greenhouse gas that has important chemical impacts on both the troposphere and the stratosphere. In the troposphere, oxidation of methane is a major regulator of OH and is a source of formaldehyde, carbon monoxide and hydrogen. In the stratosphere, CH4 plays a central role (i), due to its contribution to the stratospheric water vapor budget, and (ii), as a sink for chlorine atoms which reduces the rate of stratospheric ozone depletion. Because the different sources of methane (natural and anthropogenic like wetlands, rice paddies, termites, natural gas escape, biomass burning, etc) have distinct 13C/12C ratios (usually reported in “delta” notation δ13C), measurements of atmospheric 13CH4 content, in addition to those of the main isotopologue (12CH4), can be used to investigate individual source strengths as well as their spatial and temporal distributions. Characterization of the isotopic fractionation of methane is therefore important, for example, to help models constrain estimates of the global methane budget. However, experimental data for the 13C/12C isotope ratio are sparse. The currently accepted average value of δ13C in atmospheric methane is about -47‰ (Platt et al., 2004). The first goal of this work is to develop and to characterize (in terms of information content and error budget) an original retrieval approach to derive 13CH4 columns from ground-based Fourier transform infrared (FTIR) spectra recorded at the International Scientific Station of the Jungfraujoch (ISSJ; 46.5°N, 8.0°E, 3580m a.s.l., Swiss Alps). The retrieval strategy is based on a Tikhonov L1 approach which has been originally developed for 12CH4 by Sussmann et al. (2008) [see also contributions by Sussmann et al. to this conference (EGU2009-7869)]. In order to validate our 13CH4 products, comparisons with satellite ACE-FTS (Atmospheric Chemistry Experiment - Fourier Transform Spectrometer) measurements are performed. Then, atmospheric δ13C ratios derived from the FTIR measurements will be compared to values published in the literature and critically discussed. References: Platt, U., W. Allan and D. Lowe, Hemispheric average Cl atom concentration from 13C/12C ratios in atmospheric methane, Atmos. Chem. Phys., 4, 2393-2399, 2004. Sussmann, R., Forster, F., Borsdorff, T., et al.: Satellite validation of column-averaged methane on global scale: ground-based data from 15 FTIR stations versus last generation ENVISAT/SCIAMACHY retrievals, IGAC 10th International Conference, Annecy, France, 7-12 Sep 2008. [less ▲]

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See detailFirst measurements of the HCFC-142b trend from atmospheric chemistry experiment (ACE) solar occultation spectra
Rinsland, Curtis P; Chiou, Linda; Boone, Chris et al

in Journal of Quantitative Spectroscopy and Radiative Transfer (2009), 110(18), 2127-2134

The first measurement of the HCFC-142b (CH3CClF2) trend near the tropopause has been derived from volume mixing ratio (VMR) measurements at northern and southern hemisphere mid-latitudes for the 2004-2008 ... [more ▼]

The first measurement of the HCFC-142b (CH3CClF2) trend near the tropopause has been derived from volume mixing ratio (VMR) measurements at northern and southern hemisphere mid-latitudes for the 2004-2008 time period from spaceborne solar occultation observations recorded at 0.02 cm(-1) resolution with the ACE (atmospheric chemistry experiment) Fourier transform spectrometer. The HCFC-142b molecule is currently the third most abundant HCFC (hydrochlorofluorocarbon) in the atmosphere and ACE measurements over this time span show a continuous rise in its volume mixing ratio. Monthly average measurements at northern and southern hemisphere mid-latitudes have similar increase rates that are consistent with surface trend measurements for a similar time span. A mean northern hemisphere profile for the time span shows a near constant VMR at 8-20 km altitude range, consistent on average for the same time span with in situ results. The nearly constant vertical VMR profile also agrees with model predictions of a long lifetime in the lower atmosphere. (c) 2009 Elsevier Ltd. All rights reserved. [less ▲]

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See detailCarbonyl fluoride (COF2) vertical information above Jungfraujoch by FTIR and multi-spectra fitting: error budget and comparisons with KASIMA 3-D CTM model calculations
Duchatelet, Pierre ULiege; Mahieu, Emmanuel ULiege; Ruhnke, Roland et al

Poster (2008, April)

The major sources of fluorine in the stratosphere are CFC-11 and CFC-12. During the decomposition process, fluorine is first present in the form of carbonyl compounds (e.g. carbonyl fluoride (COF2 ... [more ▼]

The major sources of fluorine in the stratosphere are CFC-11 and CFC-12. During the decomposition process, fluorine is first present in the form of carbonyl compounds (e.g. carbonyl fluoride (COF2)). Given its long life time, COF2 is the second most abundant stratospheric fluorine reservoir. Earliest, COF2 vertical distributions were derived from occultation measurements performed by the ATMOS instrument during the SPACELAB-3 Space Shuttle mission in 1985. The Canadian FTIR spectrometer ACE-FTS, onboard the SCISAT-1 satellite, is the first instrument since the last ATMOS flight in 1994, to record COF2 vertical profiles from space. Four years of ACE-FTS occultation measurements are presently available. Several COF2 IR absorption lines located either in the so-called InSb (1-5 µm) and MCT (2-16 µm) spectral ranges can be used to determine its total column from ground-based high-resolution FTIR observations. In addition, we have proposed, during the EGU General Assembly 2007, an original retrieval procedure that allows us to derive information on the COF2 vertical distribution, between 17 and 30 km, from ground-based FTIR spectra recorded at Jungfraujoch. This “multi-microwindows multi-spectra” approach, using the SFIT-2 v3.91 algorithm, has been completely characterized in terms of fitting strategy and information content. Some examples of COF2 vertical profiles inversions were also presented. This year, we will complete the characterization of the multi-microwindows multi-spectra fitting procedure by exposing the full error budget affecting our COF2 partial and total columns products. Also, comparisons with COF2 model runs generated by the 3D CTM KASIMA (KArlsruhe SImulation model of the Middle Atmosphere) will be presented and critically discussed. [less ▲]

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See detailApproaches for retrieving abundances of methane isotopologues in the frame of the AGACC project from ground-based FTIR observations performed at the Jungfraujoch
Duchatelet, Pierre ULiege; Mahieu, Emmanuel ULiege; Demoulin, Philippe ULiege et al

Poster (2007, April)

This work has been performed within the frame of AGACC(http://www.oma.be/AGACC/Home.html), a contribution to the Belgian Scientific Support for a Sustainable Development. The project intends to make an ... [more ▼]

This work has been performed within the frame of AGACC(http://www.oma.be/AGACC/Home.html), a contribution to the Belgian Scientific Support for a Sustainable Development. The project intends to make an advanced exploitation of existing ground-based remote-sensing measurements for a selection of atmospheric species that play an important role in the chemistry of the atmosphere and that have a direct or indirect impact on climate. Target species include -among others- lower tropospheric aerosols, H2O, HDO, CH4, HCN and CO. The instrumentation includes 3 types of spectrometers (FTIR, MAXDOAS and Brewer) and one CIMEL sun photometer. These instruments are operated at 3 different sites (Jungfraujoch, Ile de la Réunion and Uccle) and most of them are affiliated with the Network for the Detection of Atmospheric Composition Change (NDACC, formerly NDSC - http://www.ndacc.org), a group dedicated to performing high-quality long-term observations. This contribution will deal with the detection of the isotopologues of methane, a species released to the atmosphere by natural processes (e.g. wetlands, termites) as well as by anthropogenic activities (e.g. fossil fuel exploitation, rice agriculture, biomass burning, etc). Due to its high warming potential and its relatively long chemical lifetime, atmospheric methane is a major greenhouse gas. Methane also affects climate by influencing tropospheric ozone and stratospheric water. The cycle of methane is complex and a thoroughly study of the sources and sinks of its main isotopologue, as well as the other isotopic species, is necessary to characterize it. Isotopic ratios are also useful to differentiate between various sources of atmospheric methane. To study the vertical distribution of methane isotopologues from the high resolution FTIR spectra recorded by the University of Liège instrument at the International Scientific Station of the Jungfraujoch (ISSJ; 46.5°N, 8.0°E, 3580m a.s.l., Swiss Alps), we have selected several 13CH4 lines distributed in the so-called InSb (1-5 µm) and MCT (2-16 µm) spectral ranges. A set of four microwindows has also been selected for the study of CH3D. Using the SFIT-2 v3.91 algorithm, vertical column abundances as well as low-resolution vertical distributions have been retrieved, adjusted from an a priori profile defined on a 41 layers scheme and derived from ACE-FTS space observations. The information content and first preliminary retrieval results will be presented. [less ▲]

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See detailDetermination of COF2 vertical distributions above Jungfraujoch by FTIR and multi-spectra fitting
Duchatelet, Pierre ULiege; Mahieu, Emmanuel ULiege; Demoulin, Philippe ULiege et al

Poster (2007, April)

The major sources of fluorine in the stratosphere are CFC-11 and CFC-12. Photolysis of these compounds leads to release of chlorine atoms, while the fluorine is, in a first step, present in the form of ... [more ▼]

The major sources of fluorine in the stratosphere are CFC-11 and CFC-12. Photolysis of these compounds leads to release of chlorine atoms, while the fluorine is, in a first step, present in the form of carbonyl compounds like COClF and COF2. Their further photolysis liberates fluorine atoms, which are quickly converted to HF. Given its long life time, COF2 is the second stratospheric fluorine reservoir. The first COF2 vertical distributions were derived from occultation measurements performed by the ATMOS instrument during the SPACELAB-3 Space Shuttle mission in 1985. The Canadian FTIR spectrometer ACE-FTS, onboard the SCISAT-1 satellite, is the first instrument since the last ATMOS flight in 1994, to record COF2 vertical profiles from space. All these observations show that, at mean latitudes, COF2 concentration is maximum between 30 and 35 km. Several COF2 IR absorption lines located either in the so-called InSb (1-5 µm) and MCT (2-16 µm) spectral ranges can be used to determine its total column from ground-based FTIR observations. In this context, several studies concerning the evolution of COF2 total column above various stations were published during the nineties. At this time, no study concerning the inversion of COF2 vertical distributions from ground-based FTIR spectra has been published. This report deals with the feasibility of such inversions, using, simultaneously, via the SFIT-2 v3.91 algorithm, a multi-microwindows and a multi-spectra fitting procedure. The multi-spectra method consists of combining several FTIR observations, recorded during the same day, to increase the information content. A selection of microwindows in InSb and MCT ranges, a complete discussion about the data characterization (e.g. information content) and typical examples of COF2 retrieved profiles from high resolution solar spectra recorded with the University of Liège Jungfraujoch FTS will be revealed. [less ▲]

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