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See detailValidation of SCIAMACHY CH4 scientific products using ground-based FTIR measurements
Dils, Bart; De Mazière, Martine; Vigouroux, Corinne et al

Poster (2008, September)

In the framework of the past EVERGREEN project, the development of three scientific algorithms, namely WFM-DOAS (henceforward called WFMD), IMAP-DOAS (henceforward called IMAP) and IMLM, commenced in ... [more ▼]

In the framework of the past EVERGREEN project, the development of three scientific algorithms, namely WFM-DOAS (henceforward called WFMD), IMAP-DOAS (henceforward called IMAP) and IMLM, commenced in order to retrieve the total column amounts of key atmospheric trace gases, including CH4, from SCIAMACHY nadir observations in its near-infrared channels. Since then, the retrieval products of these three algorithms, have undergone serious improvements. At key phases in their development, the products have been validated by using a network of ground-based FTIR instruments. Parallel with the improved SCIAMACHY data, the FTIR groups have taken steps to optimise and harmonise their own datasets and as such the different validation efforts always used the state-of-the-art FTIR dataset. Here we present an overview of the evolution of the CH4 algorithms by re-validating the data, using the same FTIR dataset (as developed under the UFTIR project) for all algorithm versions. [less ▲]

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See detailSatellite validation of column-averaged methane on global scale: ground-based data from 15 FTIR stations versus last generation ENVISAT/SCIAMACHY retrievals
Sussmann, Ralf; Foster, Frank; Borsdorff, Tobias et al

Poster (2008, September)

Previous work has shown that the precision of ground-based mid-infrared (MIR) FTIR spectrometry is sufficient to detect day-to-day variability of columnar methane, while first retrievals from ENVISAT ... [more ▼]

Previous work has shown that the precision of ground-based mid-infrared (MIR) FTIR spectrometry is sufficient to detect day-to-day variability of columnar methane, while first retrievals from ENVISAT/SCIAMACHY (channel 8) satellite measurements were impacted by a significant time-dependent bias due to detector icing. This prevented insight into true methane temporal variability at that time. The goal of our updated study is to investigate the precision of the last generation (channel 6) SCIAMACHY retrievals IMAP-DOAS v49 and WFM-DOAS v1.0 in comparison to retrievals from ground-based MIR measurements of the European FTIR network. We first briefly discuss the origin and magnitude of the natural variability of columnar methane. Subsequently, our study investigates all factors which can be optimized to improve precision of ground-based MIR-FTIR retrievals of columnar methane. This includes an optimized Tikhonov-type regularization tuned in a way to minimize the diurnal variability of retrieved columnar methane. We also discuss ways to select and average individual-pixel satellite data in order to reflect true day-to-day variability and make them comparable to ground-based data. [less ▲]

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See detailValidation of ACE-FTS N2O measurements
Strong, Kimberley; Wolff, Mareile A; Kerzenmacher, Tobias E et al

in Atmospheric Chemistry and Physics (2008), 8(16), 4759-4786

The Atmospheric Chemistry Experiment (ACE), also known as SCISAT, was launched on 12 August 2003, carrying two instruments that measure vertical profiles of atmospheric constituents using the solar ... [more ▼]

The Atmospheric Chemistry Experiment (ACE), also known as SCISAT, was launched on 12 August 2003, carrying two instruments that measure vertical profiles of atmospheric constituents using the solar occultation technique. One of these instruments, the ACE Fourier Transform Spectrometer (ACE-FTS), is measuring volume mixing ratio (VMR) profiles of nitrous oxide (N2O) from the upper troposphere to the lower mesosphere at a vertical resolution of about 3-4 km. In this study, the quality of the ACE-FTS version 2.2 N2O data is assessed through comparisons with coincident measurements made by other satellite, balloon-borne, aircraft, and ground-based instruments. These consist of vertical profile comparisons with the SMR, MLS, and MIPAS satellite instruments, multiple aircraft flights of ASUR, and single balloon flights of SPIRALE and FIRS-2, and partial column comparisons with a network of ground-based Fourier Transform InfraRed spectrometers (FTIRs). Between 6 and 30 km, the mean absolute differences for the satellite comparisons lie between -42 ppbv and +17 ppbv, with most within +/- 20 ppbv. This corresponds to relative deviations from the mean that are within +/- 15%, except for comparisons with MIPAS near 30 km, for which they are as large as 22.5%. Between 18 and 30 km, the mean absolute differences for the satellite comparisons are generally within +/- 10 ppbv. From 30 to 60 km, the mean absolute differences are within +/- 4 ppbv, and are mostly between -2 and +1 ppbv. Given the small N2O VMR in this region, the relative deviations from the mean are therefore large at these altitudes, with most suggesting a negative bias in the ACE-FTS data between 30 and 50 km. In the comparisons with the FTIRs, the mean relative differences between the ACE-FTS and FTIR partial columns (which cover a mean altitude range of 14 to 27 km) are within +/- 5.6% for eleven of the twelve contributing stations. This mean relative difference is negative at ten stations, suggesting a small negative bias in the ACE-FTS partial columns over the altitude regions compared. Excellent correlation (R=0.964) is observed between the ACE-FTS and FTIR partial columns, with a slope of 1.01 and an intercept of -0.20 on the line fitted to the data. [less ▲]

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See detailWater vapor line parameters: Some feedback from atmospheric users
Fally, Sophie; Vandaele, A. C.; Trabelsi, Samy et al

in Proceedings of the "8th Atmospheric Spectroscopy Applications" meeting (ASA2008) (2008, August)

Despite recent major improvements of water vapour databases, the insufficient quality or consistency of the H2O spectroscopic parameters has been reported many times and line parameters are often manually ... [more ▼]

Despite recent major improvements of water vapour databases, the insufficient quality or consistency of the H2O spectroscopic parameters has been reported many times and line parameters are often manually adjusted to minimize residuals and improve the quality of the fits. Atmospheric observations allow assessing the quality of databases through their simulation using the different line parameters reported in those databases. This work presents four concrete examples of the spectroscopic problems and proposed improvements in various spectral regions. [less ▲]

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See detailImpact of different spectroscopic datasets on CH4 retrievals from Jungfraujoch FTIR spectra
Duchatelet, Pierre ULg; Mahieu, Emmanuel ULg; Demoulin, Philippe ULg et al

Poster (2008, August)

Methane (CH4) is released in 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 ... [more ▼]

Methane (CH4) is released in 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 (~9 years), atmospheric methane plays a major role in the radiative forcing responsible of the greenhouse effect. Methane also affects climate by influencing tropospheric ozone and stratospheric water. The cycle of methane is complex and to understand it requires a complete study of its emissions and its budget of sources and sinks. High quality methane data sets are needed to perform such studies. CH4 vertical distributions as well as total and partial column time series can be retrieved from high-resolution ground-based FTIR spectra, using, e.g., the SFIT-2 algorithm which implements the Optimal Estimation Method of Rodgers. A set of 5 microwindows - located in the 2 to 5.5 µm range and jointly adopted by all partners involved in the European HYMN project (www.knmi.nl/samenw/hymn/) - are fitted simultaneously during the retrieval procedure. Although this approach provides relatively high information content, CH4 retrieved profiles very often present large oscillations in the troposphere, which might result partly from inappropriate or inconsistent spectroscopic parameters. Significant improvements on retrieval quality could be reached by using more accurate CH4 spectroscopic parameters. This contribution compares 3 different sets of CH4 spectroscopic parameters (including HITRAN 2004 and 2 versions where HITRAN 2004 have been updated by recent laboratory measurements), which have been tested using one year of high resolution FTIR solar observations performed at the International Scientific Station of the Jungfraujoch (Swiss Alps, 46.5°N, 8.0 °E, 3580m a.s.l.). The impact of these different spectroscopic datasets on retrieved CH4 partial columns and vertical profiles, as well as on the fitting quality (residuals) and on the error budget characterizing our CH4 products will be evaluated and discussed. [less ▲]

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See detailValidation of HNO3, ClONO2, and N2O5 from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS)
Wolff, Mareile; Kerzenmacher, Tobias; Strong, Kimberley et al

in Atmospheric Chemistry and Physics (2008), 8(13), 3529-3562

The Atmospheric Chemistry Experiment (ACE) satellite was launched on 12 August 2003. Its two instruments measure vertical profiles of over 30 atmospheric trace gases by analyzing solar occultation spectra ... [more ▼]

The Atmospheric Chemistry Experiment (ACE) satellite was launched on 12 August 2003. Its two instruments measure vertical profiles of over 30 atmospheric trace gases by analyzing solar occultation spectra in the ultraviolet/visible and infrared wavelength regions. The reservoir gases HNO3, ClONO2, and N2O5 are three of the key species provided by the primary instrument, the ACE Fourier Transform Spectrometer (ACE-FTS). This paper describes the ACE-FTS version 2.2 data products, including the N2O5 update, for the three species and presents validation comparisons with available observations. We have compared volume mixing ratio (VMR) profiles of HNO3, ClONO2, and N2O5 with measurements by other satellite instruments (SMR, MLS, MIPAS), aircraft measurements (ASUR), and single balloon-flights (SPIRALE, FIRS-2). Partial columns of HNO3 and ClONO2 were also compared with measurements by ground-based Fourier Transform Infrared (FTIR) spectrometers. Overall the quality of the ACE-FTS v2.2 HNO3 VMR profiles is good from 18 to 35 km. For the statistical satellite comparisons, the mean absolute differences are generally within ±1 ppbv ±20%) from 18 to 35 km. For MIPAS and MLS comparisons only, mean relative differences lie within±10% between 10 and 36 km. ACE-FTS HNO3 partial columns (~15–30 km) show a slight negative bias of −1.3% relative to the ground-based FTIRs at latitudes ranging from 77.8° S–76.5° N. Good agreement between ACE-FTS ClONO2 and MIPAS, using the Institut für Meteorologie und Klimaforschung and Instituto de Astrofísica de Andalucía (IMK-IAA) data processor is seen. Mean absolute differences are typically within ±0.01 ppbv between 16 and 27 km and less than +0.09 ppbv between 27 and 34 km. The ClONO2 partial column comparisons show varying degrees of agreement, depending on the location and the quality of the FTIR measurements. Good agreement was found for the comparisons with the midlatitude Jungfraujoch partial columns for which the mean relative difference is 4.7%. ACE-FTS N2O5 has a low bias relative to MIPAS IMK-IAA, reaching −0.25 ppbv at the altitude of the N2O5 maximum (around 30 km). Mean absolute differences at lower altitudes (16–27 km) are typically −0.05 ppbv for MIPAS nighttime and ±0.02 ppbv for MIPAS daytime measurements. [less ▲]

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See detailTechnical Note: New ground-based FTIR measurements at Ile de La Réunion: observations, error analysis, and comparisons with independent data
Senten, Cindy; De Mazière, Martine; Dils, Bart et al

in Atmospheric Chemistry and Physics (2008), 8(13), 3483-3508

Ground-based high spectral resolution Fourier-transform infrared (FTIR) solar absorption spectroscopy is a powerful remote sensing technique to obtain information on the total column abundances and on the ... [more ▼]

Ground-based high spectral resolution Fourier-transform infrared (FTIR) solar absorption spectroscopy is a powerful remote sensing technique to obtain information on the total column abundances and on the vertical distribution of various constituents in the atmosphere. This work presents results from two FTIR measurement campaigns in 2002 and 2004, held at Ile de La Réunion (21° S, 55° E). These campaigns represent the first FTIR observations carried out at a southern (sub)tropical site. They serve the initiation of regular, long-term FTIR monitoring at this site in the near future. To demonstrate the capabilities of the FTIR measurements at this location for tropospheric and stratospheric monitoring, a detailed report is given on the retrieval strategy, information content and corresponding full error budget evaluation for ozone (O3), methane (CH4), nitrous oxide (N2O), carbon monoxide (CO), ethane (C2H6), hydrogen chloride (HCl), hydrogen fluoride (HF) and nitric acid (HNO3) total and partial column retrievals. Moreover, we have made a thorough comparison of the capabilities at sea level altitude (St.-Denis) and at 2200 m a.s.l. (Maïdo). It is proved that the performances of the technique are such that the atmospheric variability can be observed, at both locations and in distinct altitude layers. Comparisons with literature and with correlative data from ozone sonde and satellite (i.e., ACE-FTS, HALOE and MOPITT) measurements are given to confirm the results. Despite the short time series available at present, we have been able to detect the seasonal variation of CO in the biomass burning season, as well as the impact of particular biomass burning events in Africa and Madagascar on the atmospheric composition above Ile de La Réunion. We also show that differential measurements between St.-Denis and Maïdo provide useful information about the concentrations in the boundary layer. [less ▲]

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See detailMeasured and modeled trends of stratospheric Cly and Fy column amounts in the northern hemisphere
Ruhnke, Roland; Blumenstock, Thomas; Borsdorff, Tobias et al

Poster (2008, July)

The german HGF virtual institute PEP (Pole-Equator-Pole) has been established in 2004 in order to investigate the variability of atmospheric trace constituents along a north-south transection. Within PEP ... [more ▼]

The german HGF virtual institute PEP (Pole-Equator-Pole) has been established in 2004 in order to investigate the variability of atmospheric trace constituents along a north-south transection. Within PEP the HGF centres AWI and FZK as well as the german Universities of Bremen, Karlsruhe and Potsdam combine their knowledge and capabilities in ground-based measurements and global and regional modelling of atmospheric trace constituents and aerosols. Here we present results of long-term measurements of the stratospheric column of HCl, ClONO2, HF, and O3 obtained at the different PEP stations in the northern hemisphere and in addtion at Jungfraujoch. All stations are affiliated to the NDACC (Network for the Detection of Atmospheric Composition Change). The measured time series are compared with long-term model calculations performed with a state of the art 2-D model of the University of Bremen and the 3-D CTM KASIMA. Please note, that the lowest altitude for the determination of the total columns is about 7 km leading to a slight underestimation w.r.t. the measurements. [less ▲]

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See detailCO measurements from the ACE-FTS satellite instrument: data analysis and validation using ground-based, airborne and spaceborne observations
Clerbaux, Catherine; George, Maya; Turquety, Solène et al

in Atmospheric Chemistry and Physics (2008), 8

The Atmospheric Chemistry Experiment (ACE) mission was launched in August 2003 to sound the atmosphere by solar occultation. Carbon monoxide (CO), a good tracer of pollution plumes and atmospheric ... [more ▼]

The Atmospheric Chemistry Experiment (ACE) mission was launched in August 2003 to sound the atmosphere by solar occultation. Carbon monoxide (CO), a good tracer of pollution plumes and atmospheric dynamics, is one of the key species provided by the primary instrument, the ACE-Fourier Transform Spectrometer (ACE-FTS). This instrument performs measurements in both the CO 1-0 and 2-0 ro-vibrational bands, from which vertically resolved CO concentration profiles are retrieved, from the mid-troposphere to the thermosphere. This paper presents an updated description of the ACE-FTS version 2.2 CO data product, along with a comprehensive validation of these profiles using available observations (February 2004 to December 2006). We have compared the CO partial columns with ground-based measurements using Fourier transform infrared spectroscopy and millimeter wave radiometry, and the volume mixing ratio profiles with airborne (both high-altitude balloon flight and airplane) observations. CO satellite observations provided by nadir-looking instruments (MOPITT and TES) as well as limb-viewing remote sensors (MIPAS, SMR and MLS) were also compared with the ACE-FTS CO products. We show that the ACE-FTS measurements provide CO profiles with small retrieval errors (better than 5% from the upper troposphere to 40 km, and better than 10% above). These observations agree well with the correlative measurements, considering the rather loose coincidence criteria in some cases. Based on the validation exercise we assess the following uncertainties to the ACE-FTS measurement data: better than 15% in the upper troposphere (8–12 km), than 30% in the lower stratosphere (12–30 km), and than 25% from 30 to 100 km. [less ▲]

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See detailValidation of ACE-FTS v2.2 methane profiles from the upper troposphere to the lower mesosphere
De Mazière, Martine; Vigouroux, Corinne; Bernath, Peter et al

in Atmospheric Chemistry and Physics (2008), 9(9), 2421-2435

The ACE-FTS (Atmospheric Chemistry Experiment – Fourier Transform Spectrometer) solar occultation instrument that was launched onboard the Canadian SCISAT-1 satellite in August 2003 is measuring vertical ... [more ▼]

The ACE-FTS (Atmospheric Chemistry Experiment – Fourier Transform Spectrometer) solar occultation instrument that was launched onboard the Canadian SCISAT-1 satellite in August 2003 is measuring vertical profiles from the upper troposphere to the lower mesosphere for a large number of atmospheric constituents. Methane is one of the key species. The version v2.2 data of the ACE-FTS CH4 data have been compared to correlative satellite, balloon-borne and ground-based Fourier transform infrared remote sensing data to assess their quality. The comparison results indicate that the accuracy of the data is within 10% in the upper troposphere – lower stratosphere, and within 25% in the middle and higher stratosphere up to the lower mesosphere (<60 km). The observed differences are generally consistent with reported systematic uncertainties. ACE-FTS is also shown to reproduce the variability of methane in the stratosphere and lower mesosphere. [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 ULg; Mahieu, Emmanuel ULg; 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 detailObservations of long-lived anthropogenic halocarbons at the high-Alpine site of Jungfraujoch (Switzerland) for assessment of trends and European sources
Reimann, Stefan; Vollmer, M. K.; Folini, Doris et al

in Science of the Total Environment (2008), 391

Anthropogenic halocarbons, such as chlorofluorocarbons (CFCs), hydrochlorofluorocarbons (HCFCs), hydrofluorocarbons (HFCs), bromocarbons (halons) and long-lived chlorinated solvents have been measured ... [more ▼]

Anthropogenic halocarbons, such as chlorofluorocarbons (CFCs), hydrochlorofluorocarbons (HCFCs), hydrofluorocarbons (HFCs), bromocarbons (halons) and long-lived chlorinated solvents have been measured continuously at the high-Alpine site of Jungfraujoch (Switzerland) since January 2000. Chloro- and bromo-containing halocarbons are responsible for the stratospheric ozone depletion and will be globally banned from usage within the next years. With the exception of the stable CFC-12 (CF2Cl2), all major CFCs and chlorinated solvents show a negative trend in recent years in their background concentrations at Jungfraujoch. HCFCs, as their first-generation substitute, are still increasing with a few percent per year. However, the frequency and the strength of HCFCs pollution events, which are caused by regional European emissions, are already declining. This can be seen as a sign of the impending ban of these gases within the next years in Europe. On the other hand, HFCs as the second-generation substitutes, are increasing with relative rates of at least 10% per year (e.g. almost 5 ppt per year for HFC-134a). An allocation of European sources was attempted by combining measured concentrations with trajectories of air masses reaching the Jungfraujoch during pollution events. Potential source regions could be detected in Italy, France, Spain and Germany. [less ▲]

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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 detailH2O retrievals from Jungfraujoch infrared spectra: some spectroscopic problems.
Demoulin, Philippe ULg; Trabelsi, Samy; Mahieu, Emmanuel ULg et al

in Proceedings of the 8th Atmospheric Spectroscopy Applications Meeting (2008)

Since 1949, solar absorption spectra have been acquired at the Jungfraujoch observatory (Swiss Alps, 46.5°N, 8.0°E, 3580 m a.s.l.), first with grating spectrometers, then with Fourier transform infrared ... [more ▼]

Since 1949, solar absorption spectra have been acquired at the Jungfraujoch observatory (Swiss Alps, 46.5°N, 8.0°E, 3580 m a.s.l.), first with grating spectrometers, then with Fourier transform infrared (FTIR) spectrometers. Most observations collected with these instruments encompass water vapor absorptions, even the narrow spectral domains regularly recorded with the grating instruments to monitor the evolution of important atmospheric constituents. The aim of this work is to analyze all available spectra containing usable H2O absorption lines, to derive a long-term record of its total column in the atmosphere above the Jungfraujoch. In addition, more recent FTIR broadband spectra, with better signal-to-noise ratio and resolution, will be analyzed with state of the art algorithm, in order to derive information on the vertical distribution of H2O. [less ▲]

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See detailGround-based CO observations at the Jungfraujoch: Comparison between FTIR and NDIR measurements
Dils, Bart; Mahieu, Emmanuel ULg; Demoulin, Philippe ULg et al

in Geophysical Research Abstracts (2008), 10

Measurements of CO have been performed at the Swiss Alpine Jungfraujoch station (46.5º N, 8.0° E, 3580m a.s.l.) on a regular basis since the mid-1980’s, using Fourier Transform Infrared solar absorption ... [more ▼]

Measurements of CO have been performed at the Swiss Alpine Jungfraujoch station (46.5º N, 8.0° E, 3580m a.s.l.) on a regular basis since the mid-1980’s, using Fourier Transform Infrared solar absorption spectrometry (FTIR), and since 1996 using an in situ Nondispersive Infrared technique (NDIR). While the in situ measurements detect local CO concentrations at the site, the FTIR technique provides integrated measurements along the line-of-sight. Nevertheless, the pressure broadening of the spectral absorption lines recorded at high resolution enables retrieving information on the vertical distribution of CO, mainly in the troposphere, including its concentration near the surface. Considering the inherent capabilities of the two independent measurement techniques, substantial differences between both data sets for surface level CO could potentially arise. Here we present a comparison of both data sets for the 1997 -2004 time period. Both data sets have been analysed by using successive Kolmogorov-Zurbenko filters. It appears that the long-term trend over the given time period is significantly different for both datasets. Possible causes for this difference will be critically discussed. [less ▲]

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See detailRetrievals of C2H2 from high-resolution FTIR solar spectra recorded at the Jungfraujoch station (46.5ºN) and comparison with ACE-FTS observations
Mahieu, Emmanuel ULg; Duchatelet, Pierre ULg; Bernath, P. F. et al

in Geophysical Research Abstracts (2008), 10

Acetylene (C2H2) is among the nonmethane hydrocarbons (NMHCs) accessible to infrared remote sensing technique. As a product of combustion and biomass burning, it is emitted at the Earth’s surface and ... [more ▼]

Acetylene (C2H2) is among the nonmethane hydrocarbons (NMHCs) accessible to infrared remote sensing technique. As a product of combustion and biomass burning, it is emitted at the Earth’s surface and further transported and mixed into the troposphere. Destruction by OH is the main removal process. The average tropospheric lifetime of C2H2 is estimated at about 1 month on the global scale; at mid-latitudes, it varies between 20 days in summer to 160 days in winter. This compound is appropriate to study tropospheric pollution and transport, and is often used in conjunction with other tracers of fires. C2H2 presents exploitable infrared absorption features near 3 and 15 μm, where weak isolated lines of the nu5 and the nu2 + nu4 + nu5 bands are found, respectively. Several of these lines can be used to retrieve abundances of C2H2 from high-resolution groundbased infrared solar spectra. Typical observations recorded at the Jungfraujoch station (46.5ºN, 8.0ºE, 3580m asl, Swiss Alps) by the NDACC (Network for the Detection of Atmospheric Composition Change)-affiliated Bruker instrument have been fitted with the OEM-SFIT-2 (v3.91) algorithm. Various approaches and combination of lines have been tested, seeking for the optimum inversion strategy. The HITRAN-2004 spectroscopic line parameters including the August 2006 updates for water vapor have been adopted in the retrievals. These approaches will be presented and critically compared, with the help of error budget and information content analyses, taking into account the impact of major interferences such as water vapor. The time series of C2H2 tropospheric column abundances above Jungfraujoch will also be presented, including determination of its long-term trend and strong seasonal cycle. The ground-based results will further be compared with zonal mean observations performed by the ACE-FTS space-based instrument since early 2004. [less ▲]

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See detailImpact of different spectroscopic datasets on CH4 retrievals from Jungfraujoch FTIR spectra
Duchatelet, Pierre ULg; Mahieu, Emmanuel ULg; Demoulin, Philippe ULg et al

(2008)

Due to its high warming potential and its relatively long chemical lifetime (~9 years), atmospheric methane (CH4) plays a major role in the radiative forcing responsible of the greenhouse effect. Methane ... [more ▼]

Due to its high warming potential and its relatively long chemical lifetime (~9 years), atmospheric methane (CH4) plays a major role in the radiative forcing responsible of the greenhouse effect. Methane also affects climate by influencing tropospheric ozone and stratospheric water. High quality methane data sets are needed to understand its cycle and evaluate its budget of sources and sinks. Methane vertical distribution as well as total and partial column time series can be retrieved from high-resolution ground-based FTIR spectra, using, e.g., the SFIT-2 algorithm which implements the Optimal Estimation Method of Rodgers . However, although several retrieval approaches characterized by relatively high information content exist, methane retrieved profiles very often present large oscillations in their tropospheric range, which might result partly from inappropriate or inconsistent parameters. Significant improvements on retrieval quality should therefore be reached by using more accurate or compatible CH4 spectroscopic data. The main purpose of this contribution is to test and compare three different sets of CH4 spectroscopic parameters and to quantify their impact on CH4 retrieved products as well as on the fitting quality. [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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