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See detailDecrease of the Carbon Tetrachloride (CCl4) Loading above Jungfraujoch, based on High Resolution Infrared Solar Spectra recorded between 1999 and 2011
Rinsland, C. P.; Mahieu, Emmanuel ULg; Demoulin, Philippe ULg et al

in Journal of Quantitative Spectroscopy & Radiative Transfer (2012), 113

The long-term trend of the atmospheric carbon tetrachloride (CCl4) burden has been retrieved from high spectral resolution infrared solar absorption spectra recorded between January 1999 and June 2011 ... [more ▼]

The long-term trend of the atmospheric carbon tetrachloride (CCl4) burden has been retrieved from high spectral resolution infrared solar absorption spectra recorded between January 1999 and June 2011. The observations were made with a Fourier transform spectrometer at the northern mid-latitude, high altitude Jungfraujoch station in Switzerland (46.5°N latitude, 8.0°E longitude, 3580 m altitude). Total columns were derived from spectrometric analysis of the strong CCl4 ν3 band at 794 cm-1, accounting for all interfering molecules (e.g., H2O, CO2, O3, and a dozen weakly absorbing gases). A significant improvement in the fitting residuals and in the retrieved CCl4 columns was obtained by taking into account line mixing in a strong interfering CO2 Q branch. This procedure had never been implemented in remote sensing CCl4 retrievals though its importance was noted in earlier studies. A fit to the CCl4 daily mean total column time series returns a statistically-significant long-term trend of (-1.49±0.08 x 1013 molec./cm2)/yr, 2-σ. This corresponds to an annual decrease of (-1.31±0.07) pptv for the mean free tropospheric volume mixing ratio. Furthermore, the total column data set reveals a weak seasonal cycle with a peak-to-peak amplitude of 4.5 %, with minimum and maximum values occurring in mid-February and mid-September, respectively. This small seasonal modulation is attributed primarily to the residual influence of tropopause height changes throughout the year. The negative trend of the CCl4 loading reflects the continued impact of the regulations implemented by the Montreal Protocol and its strengthening amendments and adjustments. Despite this statistically significant decrease, the CCl4 molecule currently remains an important contributor to the atmospheric chlorine budget, and thus deserves further monitoring, to ensure continued compliance with these strengthenings, globally. Our present findings are briefly discussed with respect to recent relevant CCl4 investigations at the ground and from space. [less ▲]

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See detailRetrievals of ethane from ground-based high-resolution FTIR solar observations with updated line parameters: determination of the optimum strategy for the Jungfraujoch station.
Bader, Whitney ULg; Perrin, Agnès; Jacquemart, David et al

in Geophysical Research Abstracts (2012), 14(EGU2012-9126),

Ethane (C2H6) is the most abundant Non-Methane HydroCarbon (NMHC) in the Earth’s atmosphere, with a lifetime of approximately 2 months. C2H6 has both anthropogenic and natural emission sources such as ... [more ▼]

Ethane (C2H6) is the most abundant Non-Methane HydroCarbon (NMHC) in the Earth’s atmosphere, with a lifetime of approximately 2 months. C2H6 has both anthropogenic and natural emission sources such as biomass burning, natural gas loss and biofuel consumption. Oxidation by the hydroxyl radical is by far the major C2H6 sink as the seasonally changing OH concentration controls the strong modulation of the ethane abundance throughout the year. Ethane lowers Cl atom concentrations in the lower stratosphere and is a major source of peroxyacetyl nitrate (PAN) and carbon monoxide (by reaction with OH). Involved in the formation of tropospheric ozone and in the destruction of atmospheric methane through changes in OH, C2H6 is a non-direct greenhouse gas with a net-global warming potential (100-yr horizon) of 5.5. The retrieval of ethane from ground-based infrared (IR) spectra is challenging. Indeed, the fitting of the ethane features is complicated by numerous interferences by strong water vapor, ozone and methane absorptions. Moreover, ethane has a complicated spectrum with many interacting vibrational modes and the current state of ethane parameters in HITRAN (e.g. : Rothman et al., 2009, see http://www.hitran.com) was rather unsatisfactory in the 3 µm region. In fact, PQ branches outside the 2973–3001 cm-1 range are not included in HITRAN, and most P and R structures are missing. New ethane absorption cross sections recorded at the Molecular Spectroscopy Facility of the Rutherford Appleton Laboratory (Harrison et al., 2010) are used in our retrievals. They were calibrated in intensity by using reference low-resolution spectra from the Pacific Northwest National Laboratory (PNNL) IR database. Pseudoline parameters fitted to these ethane spectra have been combined with HITRAN 2004 line parameters (including all the 2006 updates) for all other species encompassed in the selected microwindows. Also, the improvement brought by the update of the line positions and intensities of methyl chloride (CH3Cl) in the 3.4 m region (Bray et al., 2011) will be quantified. The ethane a priori volume mixing ratio (VMR) profile and associated covariance are based on synthetic data from the chemical transport model (CTM) of the University of Oslo. In this contribution, we will present updated ethane total and tropospheric column retrievals, using the SFIT-2 algorithm (v3.91) and high-resolution Fourier Transform Infrared (FTIR) solar absorption observations recorded with a Bruker 120HR instrument, at the high altitude research station of the Jungfraujoch (46.5°N, 8°E, 3580 m asl), within the framework of the Network for the Detection of Atmospheric Composition Change (NDACC, visit http://www.ndacc.org). We will characterize three microwindows encompassing the strongest ethane features after careful selection of a priori VMR profiles, spectroscopic parameters, accounting at best for all interfering species. We will then present the retrieval strategy representative of the best combination of those three characterized micro-windows in order to minimize the fitting residuals while maximizing the information content, the precision and the reliability of the retrieved product. The long-term C2H6 column time series will be produced using the Jungfraujoch observational database. Comparisons with synthetic data produced by two chemical transport model (CHASER and the one of the University of Oslo) will also be presented and analyzed, aiming at the determination and interpretation of long-term trends and interannual variations of ethane at Northern mid-latitudes. [less ▲]

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See detailLong-term series of tropospheric water vapour amounts and HDO/H2O ratio profiles above Jungfraujoch
Lejeune, Bernard ULg; Mahieu, Emmanuel ULg; Schneider, Matthias et al

in Geophysical Research Abstracts (2012), 14

Water vapour is a crucial climate variable involved in many processes which widely determine the energy budget of our planet. In particular, water vapour is the dominant greenhouse gas in the Earth’s ... [more ▼]

Water vapour is a crucial climate variable involved in many processes which widely determine the energy budget of our planet. In particular, water vapour is the dominant greenhouse gas in the Earth’s atmosphere and its radiative forcing is maximum in the middle and upper troposphere. Because of the extremely high variability of water vapour concentration in time and space, it is challenging for the available relevant measurement techniques to provide a consistent data set useful for trend analyses and climate studies. Schneider et al. (2006a) showed that ground-based Fourier Transform Infrared (FTIR) spectroscopy, performed from mountain observatories, allows for the detection of H2O variabilities up to the tropopause. Furthermore, the FTIR measurements allow the retrieval of HDO amounts and therefore the monitoring of HDO/H2O ratio profiles whose variations act as markers for the source and history of the atmospheric water vapour. In the framework of the MUSICA European project (Multi-platform remote Sensing of Isotopologues for investigating the Cycle of Atmospheric water, http://www.imk-asf.kit.edu/english/musica.php), a new approach has been developed and optimized by M. Schneider and F. Hase, using the PROFFIT algorithm, to consistently retrieve tropospheric water vapour profiles from high-resolution ground-based infrared solar spectra and so taking benefit from available long-term data sets of ground-based observations. The retrieval of the water isotopologues is performed on a logarithmic scale from 14 micro-windows located in the 2600-3100 cm-1 region. Other important features of this new retrieval strategy are: a speed dependant Voigt line shape model, a joint temperature profile retrieval and an interspecies constraint for the HDO/H2O profiles. In this contribution, we will combine the quality of the MUSICA strategy and of our observations, which are recorded on a regular basis with FTIR spectrometers, under clear-sky conditions, at the NDACC site (Network for the Detection of Atmospheric Composition Change, http://www.ndacc.org) of the Jungfraujoch International Scientific Station (Swiss Alps, 46.5°N, 8.0°E, 3580m asl). Information content analysis of the retrieved H2O products allows us to produce a long-term trend from 1996 to 2011 for different tropospheric levels. We will compare the annual cycle of tropospheric HDO/H2O ratio profiles with those already produced at other sites (Schneider et al., 2010). We will also focus on the diurnal variability of water vapour to determine a time limit in the inter-comparison of different water vapour measurement techniques. [less ▲]

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See detailLong-term trends of a dozen direct greenhouse gases derived from infrared solar absorption spectra recorded at the Jungfraujoch station
Mahieu, Emmanuel ULg; Duchatelet, Pierre; Zander, Rodolphe ULg et al

Poster (2011, November 10)

References Bader, W. et al., Extension of the long-term total column time series of atmospheric methane above the Jungfraujoch station: analysis of grating infrared spectra between 1976 and 1989 ... [more ▼]

References Bader, W. et al., Extension of the long-term total column time series of atmospheric methane above the Jungfraujoch station: analysis of grating infrared spectra between 1976 and 1989, Geophysical Research Abstracts, 13, EGU2011-3391-1, 2011. [http://hdl.handle.net/2268/88180] Duchatelet, P. et al., First retrievals of carbon tetrafluoride (CF4) from ground-based FTIR measurements: production and analysis of the two-decadal time series above the Jungfraujoch, Geophysical Research Abstracts, 13, EGU2011-6413, 2011. [http://hdl.handle.net/2268/90745] Gardiner, T. et al., Trend analysis of greenhouse gases over Europe measured by a network of ground-based remote FTIR instruments, Atmos. Chem. Phys., 8, 6719-6727, 2008. [http://hdl.handle.net/2268/2545] Rodgers, C.D., Characterisation and error analysis of profiles derived from remote sensing measurements, J. Geophys. Res., 95, 5587-5595, 1990. Zander, R. et al., Our changing atmosphere: Evidence based on long-term infrared solar observations at the Jungfraujoch since 1950, Sci. Total Environ., 391, 184-195, 2008. [http://hdl.handle.net/2268/2421] [less ▲]

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See detailAnalysis of historical grating spectra: Jungfraujoch atmospheric database extended back to 1977
Demoulin, Philippe ULg; Roland, Ginette; Bader, Whitney ULg et al

Conference (2011, November 10)

Historical solar spectra recorded at the Jungfraujoch station with a high-resolution grating spectrometer have been re-analyzed to derive total columns of a series of atmospheric gases. This instrument ... [more ▼]

Historical solar spectra recorded at the Jungfraujoch station with a high-resolution grating spectrometer have been re-analyzed to derive total columns of a series of atmospheric gases. This instrument, built and operated by the University of Liège (Belgium), was used in the Sixties and Seventies to record two solar spectrum atlases extending from the near-UV to the near-IR. From 1977 to 1989, it was also regularly used to record narrow spectral intervals in the mid-infrared, encompassing absorption lines of gases of atmospheric interest, e.g. CH4, HF, HCl, H2O, N2O, NO2, C2H6, O3 and CO. More than 10 thousand spectra were recorded during this period. The total columns derived from these grating spectra have been combined with the FTIR columns derived at the Jungfraujoch since the mid-1980s, in order to derive the temporal evolution of various target gases for the period 1977-2011. [less ▲]

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See detailComparisons of long-term stratospheric nitric acid and hydrogen fluoride variations using satellite and ground-based measurements
Froidevaux, L.; Anderson, J.; Hannigan, J. et al

Conference (2011, November 09)

We investigate the long-term variations of stratospheric nitric acid (HNO3) and hydrogen fluoride (HF), based on several satellite and ground-based measurement records. We use results from the Upper ... [more ▼]

We investigate the long-term variations of stratospheric nitric acid (HNO3) and hydrogen fluoride (HF), based on several satellite and ground-based measurement records. We use results from the Upper Atmosphere Research Satellite (launched in late 1991 and decommissioned in late 2005), the Aura satellite (launched in summer 1991, with on-going measurements), and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) (from 2004 to present), in conjunction with several long-term ground-based datasets from the Network for the Detection of Atmosphere Composition Change (NDACC). In particular, we investigate the time series of HNO3 and HF, using NDACC column data for validation. We focus here on a few NDACC sites with long-term and frequent measurements, namely the Jungfraujoch (45N, 8E), Lauder (45S, 170E), and Mauna Loa (20N, 204E) sites, where ground-based Fourier Transform Infrared (FTIR) measurements have covered both the UARS and Aura time periods (1991 to present). For HNO3, we investigate whether there are indications of a systematic offset between the measurements by the Microwave Limb Sounder (MLS) instruments aboard both UARS and Aura. For hydrogen fluoride, the HALogen Occultation Experiment's HF time series are connected to the ACE-FTS dataset, and we analyze the correlation of this time series with the ground-based datasets. In addition, model runs from the Whole Atmosphere Community Climate Model (WACCM) and the TOMCAT/SLIMCAT model are used as part of the long-term time series intercomparisons. We note that there is a significant time gap in the HNO3 time series from the satellite measurements used here. The long-term satellite datasets studied here include zonal average Earth Science Data Records (ESDRs) being produced under the Global Ozone Chemistry And Related trace gas Data records for the Stratosphere (GOZCARDS) project, part of the NASA Making Earth Science data records for Use in Research Environments (MEaSUREs) program. We also analyze coincident-type measurements, for the comparisons between satellite and ground-based observations. [less ▲]

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See detailOzone tropospheric and stratospheric trends (1995-2011) at six ground- based FTIR stations (34°S to 79°N)
Vigouroux, Corinne; Demoulin, Philippe ULg; Hase, Frank et al

Poster (2011, November)

Five ground-based stations in Western Europe, from 79°N to 28°N, all part of the Network for the Detection of Atmospheric Composition Change (NDACC), have joined their efforts to homogenize and optimize ... [more ▼]

Five ground-based stations in Western Europe, from 79°N to 28°N, all part of the Network for the Detection of Atmospheric Composition Change (NDACC), have joined their efforts to homogenize and optimize the retrievals of ozone profiles from FTIR (Fourier transform infrared) solar absorption spectra. Using the optimal estimation method, distinct vertical information can be obtained in four layers: ground—10 km, 10—18 km, 18—27 km, and 27—42 km, in addition to total column amounts. A bootstrap resampling method has been implemented to determine annual partial and total column trends. Vigouroux et al. (2008) applied this method to the ozone data and discussed the trends of the total columns and of the partial columns in the above four layers, over the period 1995-2004. The updated trends for the 1995-2009 period has been published in the WMO 2010 report. Here, we present the updated trends for the 1995-mid-2011 period, for the five European stations but also for a southern hemisphere station, Wollongong (34°S), which recently joined this ozone network. [less ▲]

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See detailChanges in atmospheric composition discerned from long-term NDACC measurements: trends in direct greenhouse gases derived from infrared solar absorption spectra recorded at the Jungfraujoch station
Mahieu, Emmanuel ULg; Duchatelet, Pierre ULg; Zander, Rodolphe ULg et al

Poster (2011, October 25)

The University of Liège (ULg) is operating -under clear sky conditions- two state-of-the-art Fourier Transform Infrared (FTIR) spectrometers at the high-altitude research station of the Jungfraujoch ... [more ▼]

The University of Liège (ULg) is operating -under clear sky conditions- two state-of-the-art Fourier Transform Infrared (FTIR) spectrometers at the high-altitude research station of the Jungfraujoch (Swiss Alps, 46.5ºN, 3580m asl), within the framework of the Network for the Detection of Atmospheric Composition Changes (NDACC). Routine FTIR operation started in 1984. Since then, it has been continued without disruption, allowing collecting more than 45000 high-resolution broadband IR solar absorption spectra, between 2 and 16 µm, using either HgCdTe or InSb detectors as well as a suite of optical filters. Typically, the spectral resolutions achieved lie in the 0.003 to 0.009 cm-1 interval while signal-to-noise ratios of 1000 and more are reached. Numerous narrow-band IR spectra essentially recorded from 1976 to 1989 with grating instruments are also available. Their analyses with modern tools have recently started [Bader et al., 2011] and will be pursued to consistently extend our datasets back in the 1970s. Geophysical parameters are deduced from the ULg observational database either with the SFIT-1, SFIT-2 or PROFFIT-9 algorithm, allowing producing total column time series of the target gases. In addition, information on their vertical distributions with altitude can generally be derived when using SFIT-2 or PROFFIT-9 which both implement the Optimal Estimation Method of Rodgers [1990]. Presently, more than two dozen atmospheric species are systematically retrieved from the Jungfraujoch observations, allowing the monitoring of key constituents of the Earth's atmosphere which play important roles in stratospheric ozone depletion and/or in global warming. This communication will focus on the direct and major greenhouse gases available from our database, namely water vapor, CO2, CH4, N2O, tropospheric ozone, CFC-11, CFC-12, HCFC-22, CCl4, SF6, as well as CF4 which has recently been added to our targets list [Duchatelet et al., 2011]. Trends and associated uncertainties characterizing the available -and often multi-decadal- time series have been derived or updated with a statistical bootstrap resampling tool [Gardiner et al., 2008], they will be presented and critically compared with data available from the literature. [less ▲]

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See detailScientific Assessment of Ozone Depletion: 2010, Chapter 2 - Stratospheric Ozone and Surface Ultraviolet Radiation
Douglass, A.; Fioletov, V.; Godin-Beekmann, Sophie et al

Report (2011)

As a result of the Montreal Protocol, ozone is expected to recover from the effect of ozone-depleting substances (ODSs) as their abundances decline in the coming decades. The 2006 Assessment showed that ... [more ▼]

As a result of the Montreal Protocol, ozone is expected to recover from the effect of ozone-depleting substances (ODSs) as their abundances decline in the coming decades. The 2006 Assessment showed that globally averaged column ozone ceased to decline around 1996, meeting the criterion for the first stage of recovery. Ozone is expected to increase as a result of continued decrease in ODSs (second stage of recovery). This chapter discusses recent observations of ozone and ultraviolet radiation in the context of their historical records. Natural variability, observational uncertainty, and stratospheric cooling necessitate a long record in order to attribute an ozone increase to decreases in ODSs. The primary tools used in this Assessment for prediction of ozone are chemistry-climate models (CCMs). These CCMs are designed to represent the processes determining the amount of stratospheric ozone and its response to changes in ODSs and greenhouse gases. Eighteen CCMs have been recently evaluated using a variety of process-based compari-sons to measurements. The CCMs are further evaluated here by comparison of trends calculated from measurements with trends calculated from simulations designed to reproduce ozone behavior during an observing period. [less ▲]

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See detailAdvanced exploitation of Ground-Based measurements for Atmospheric Chemistry and Climate Applications "AGACC"
De Mazière, Martine; De Backer, Hugo; Carleer, Michel et al

Report (2011)

We live in an era in which human activities are causing significant changes to the atmospheric environment which result in local to global consequences on the ecosystems. Changes in the atmospheric ... [more ▼]

We live in an era in which human activities are causing significant changes to the atmospheric environment which result in local to global consequences on the ecosystems. Changes in the atmospheric composition impact our climate via chemical and dynamical feedback mechanisms; in many instances they also affect air quality, and the health of the biosphere. Monitoring and understanding those changes and their consequences is fundamental to establish adequate actions for adaptation to and mitigation of the environmental changes. Furthermore, after implementation of regulatory measures like the Montreal Protocol, it is necessary to verify whether the measures are effective. This can only be achieved if we have adequate detection methods and a reliable long record of a series of key geophysical parameters. Thus the AGACC project contributes to the provision of basic new knowledge regarding the atmospheric composition and its changes, based on advanced groundbased monitoring, in combination with satellite and numerical modelling data. Its results are integrated in ongoing international research programmes. The general objective of AGACC has been to improve and extend the groundbased detection capabilities for a number of climate-related target species and, based hereupon, analyse past and present observations to derive new information about the atmospheric composition, its variability and long-term changes. Despite the advent of a growing and more performant fleet of Earth Observation satellites, ground-based observations are still indispensable to (1) guarantee long-term continuity, homogeneity and high quality of the data, and (2) to underpin the satellite data for calibration and (long-term) validation. A first target gas is atmospheric water vapour. It is the key trace gas controlling weather and climate. It is also the most important greenhouse gas in the Earth’s atmosphere. Its amount and vertical distribution are changing, but how and why? Especially in the upper troposphere - lower stratosphere, the radiative effects of changes in the water vapour are significant and should be quantified. The measurement of water vapour is a hot topic since several years. It is a challenge, because water vapour exhibits a large gradient in its concentration when going from the ground to the stratosphere, and because it is highly variable in time and space. For example, we have found that the time scale of the variations of the total water vapour amount at Jungfraujoch is in the order of minutes. In AGACC, we have therefore investigated various experimental techniques to measure the concentration of water vapour in the atmosphere, focusing on the total column as well as on the vertical distribution in the troposphere up to the lower stratosphere. The retrieval of water vapour vertical profiles and total columns from ground-based FTIR data has been initiated at three very different stations where correlative data for verification are available, namely Ukkel (± sea level, mid-latitude), Ile de La Réunion (± sea level, tropical) and Jungfraujoch (high altitude, mid-latitude), with promising results. In particular, at Jungfraujoch, it has been demonstrated that the precision of the FTIR integrated water vapour (IWV) measurements is of order 2%. The capability to retrieve individual isotopologues of water vapour, and to monitor their daily and diurnal variations, has also been demonstrated. This could open new ways to study in the future the role of water vapour in the radiative balance, the global circulation, precipitation etc. We also started joint exploitation of ground-based FTIR and satellite IASI data for water vapour and its isotopologues, in order to exploit fully the potential of the existing instrumentation. A correction method for the radiosoundings at Ukkel has been successfully implemented, resulting in a homogeneous and reliable time series from 1990 to 2008 from which trends in upper troposphere humidity (UTH) and tropopause characteristics have been derived. One observes a rising UTH until September 2001, followed by a decline, accompanied by a descent and heating of the tropopause up to the turning point and an ascent and cooling afterwards. The changes after September 2001 in the upper troposphere can be explained by surface heating and convective uplift. At Jungfraujoch, one does not observe any significant trend in the total water vapour abundance above the station over the 1988-2010 time period, although significant positive summer and negative winter trends have been detected. We have made a quantitative statistical comparison between ground-based FTIR, CIMEL, GPS and integrated (corrected) radio sounding measurements of the IWV at Ukkel. This work is important to better characterize the different sensors in order to exploit together different observations made by different instruments. A second target species is atmospheric aerosol. There is a very large variety of aerosol both from natural or anthropogenic origin. One of the reasons why they are so important is that they affect the optical properties of the atmosphere. In particular, it has been demonstrated in previous studies that the aerosols have a large impact on the quantity of harmful UV-B radiation received at the Earth’s surface. The latest IPCC Report also stressed that the radiative forcing caused by atmospheric aerosols is one of the largest uncertainties in determining the total radiative forcing in the atmosphere. Better monitoring capabilities of aerosol properties can therefore improve our understanding and forecasting of the atmospheric processes and evolution, and in particular of UV-B and climate changes. Several measurement techniques are now operational in the AGACC consortium for the ground-based monitoring of aerosol properties. These are the Brewer spectrometer and CIMEL observations at Ukkel, the latter contributing also to the AERONET network since July 2006, and the newly developed MAXDOAS observations. Unlike CIMEL and Brewer measurements, that provide the total Aerosol Optical Depth, it has been demonstrated that the MAXDOAS measurements also provide additional information about the vertical distribution of the aerosol extinction in the lowest kilometres of the troposphere. A better understanding of the ultimate capabilities of MAXDOAS aerosol remote sensing has been gained through participation to the international CINDI campaign (Cabauw Intercomparison Campaign of Nitrogen Dioxide measuring Instruments ) in summer 2009. The combination of Brewer, CIMEL and MAXDOAS instruments gives us a remote-sensing dataset that will enable a more comprehensive characterization of the tropospheric aerosol optical properties. The usefulness of these aerosol observations has already been demonstrated in the improvement of the UVindex predictions for the general public. Another application is their use as input data in the retrieval of vertical profiles of tropospheric pollutants from MAXDOAS measurements, like tropospheric NO2 and formaldehyde. Third we have focused on a few climate-related trace gases. Changing greenhouse gas and aerosol concentrations directly affect the radiative budget of the atmosphere, and therefore climate. But many species known as pollutants like carbon monoxide (CO), nitrogen oxides (NOx) and hydrocarbons, - often related to fossil fuel or biomass burning -, also affect climate through their role in chemical reactions that produce tropospheric ozone, which is a well-known greenhouse gas, or that modify the lifetime of gases like methane, or the oxidation capacity of the atmosphere. Therefore in AGACC, we have focused on the measurement of a number of trace gases that are subject to changing concentrations, that directly or indirectly affect climate, and that are either difficult to monitor or that have not yet been measured from the ground. We have included attempts to observe distinctly some isotopologues, because the isotopic ratios observed in an airmass provide information on its history, and because the FTIR solar absorption measurements provide a rather unique capability hereto. The investigated species are the isotopologues of CH4 and CO, and hydrogen cyanide (HCN), as examples of biomass burning tracers, some hydrocarbons like formaldehyde (HCHO), ethylene (C2H4) and acetylene (C2H2), and HCFC-142b, a replacement product for CFCs and a greenhouse gas. In many cases, retrieval strategies had to be adapted when going from one site to another with different atmospheric conditions, especially when the local humidity and abundances are very different as is the case between Jungfraujoch (dry, high altitude, mid-latitude) and Ile de La Réunion (humid, low altitude, low latitude). Still we have been able to show the feasibility of retrieving particular trace gas information even under difficult conditions. Many of our results have been compared to correlative data, to validate the approach and to gain complementary information. It is also important to note that the retrieval strategies developed in AGACC have regularly been presented to the global Network for the Detection of Atmospheric Composition Change (NDACC) UV-Vis and Infrared communities and have often been adopted by others or even proposed for adoption as a standard in the community (e.g., for hydrogen cyanide (HCN)). In particular: We have been able to study the seasonal variations of HCN at the Jungfraujoch and at Ile de La Réunion, and to show the dominant impact of biomass burning. Formaldehyde was studied in much detail at Ukkel, Jungfraujoch and Ile de la Réunion. The challenge for detection at Jungfraujoch is the small abundance (about 10 times smaller than at Ukkel and Ile de La Réunion); a particular observation strategy was developed successfully, resulting in a time series that already shows the day-to-day and seasonal variations. At Ile de La Réunion, comparisons of FTIR, MAXDOAS, satellite and model data have (1) shown the good agreement between the various data sets, but also, (2), the variability of HCHO (diurnal, seasonal, day-to-day), and (3), thanks to the complementarities of the various data sets, they have enabled us to learn more about the long-range transport of Non-methane Volatile Organic Compounds (NMVOCS, precursors of HCHO) and deficiencies in the models. It was shown that fast, direct transport of NMVOCS from Madagascar has a significant impact on the HCHO abundance and its variability at Ile de La Réunion, and that this is underestimated in the model. Significant progress was made as to the detection of 13CH4 and CH3D from ground-based FTIR observations, both at Jungfraujoch and Ile de La Réunion. To our knowledge, it is the first time that a d13C data set is derived from ground-based FTIR observations. More work is needed to improve the CH3D retrieval at Ile de La Réunion, and to interpret the results, in combination with models. Also for the first time, 12CO and 13CO have been retrieved individually at Jungfraujoch. The d13C time series shows significant seasonal and interannual changes. As to the hydrocarbon ethylene, it is shown that it can be detected at Jungfraujoch only in spectra at low solar elevation, given its small atmospheric abundance. Regarding acetylene, the observed time series at Jungfraujoch and Ile de La Réunion show clear seasonal variations and enhancements due to the impact of biomass burning events, correlated with enhancements in CO, C2H6 and HCN. It is not clear yet whether we can reliably retrieve the concentration of HCFC- 142b, a replacement product that is increasing strongly in the troposphere. New line parameters for the interfering species HFC-134a are required to confirm/infirm the preliminary results. This highlights again the importance of the laboratory work for providing such parameters. Improved line parameters have been obtained for water vapour and its isotopologues, ethylene and formic acid. These AGACC results have been integrated in the international spectroscopic databases. We also showed that line intensities available around 2096 cm–1 for the 13C16O isotopologue of carbon monoxide in the HITRAN database seem to be accurate to 2%. We failed to improve line intensities for the 13.6 μm region of acetylene. The new data sets that have been derived in AGACC from FTIR and MAXDOAS observations have been archived in the NDACC data centre, where they are available for users (generally modelers and satellite teams). In addition, they are stored locally and are available to users upon request. AGACC results have been reported to the international scientific community, via the literature, via integration in geophysical or spectroscopic databases, and via participation to international research initiatives like the Atmospheric Water Vapour in the Climate System (WAVACS) Cost Action, the International Space Science Institute (ISSI) Working Group on Atmospheric Water Vapour, the International Union of Pure and Applied Chemistry (IUPAC) project, the International CINDI campaign, etc. The results have already found important scientific applications. A few examples are worth mentioning: the re-evaluation of methane emissions in the tropics from SCIAMACHY based on the new H2O spectroscopy, and the improved retrievals of HCOOH from the satellite experiments ACE-FTS and IASI, and from the ground. In the longer-term, the AGACC results will no doubt benefit the research in atmospheric sciences –in particular in the monitoring of its composition changes–, which is the fundamental basis of environmental assessment reports for supporting policy makers. [less ▲]

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See detailExtension of the long-term total column time series of atmospheric methane above the Jungfraujoch station: analysis of grating infrared spectra between 1976 and 1989
Bader, Whitney ULg; Lejeune, Bernard ULg; Demoulin, Philippe ULg et al

in Geophysical Research Abstracts (2011), 13

Methane (CH4) is one of the most abundant greenhouse gases in the Earth’s atmosphere, with current mean volume mixing ratio close to 1800 ppb. Since methane has a global warming potential of 25 (100-yr ... [more ▼]

Methane (CH4) is one of the most abundant greenhouse gases in the Earth’s atmosphere, with current mean volume mixing ratio close to 1800 ppb. Since methane has a global warming potential of 25 (100-yr horizon) and an atmospheric lifetime of 12 years, the Kyoto Protocol has included it among the species to be regulated to limit global warming. Anthropogenic sources of methane are mainly energy production (coal and leaks) and agriculture while main natural sources are swamps and biomass waste. The main sink of methane is oxidation in the troposphere, primarily by reaction with the hydroxyl radical. Methane trends have exhibited significant changes during the last twenty-five years. For instance, long-term monitoring of its vertical total column above the high-altitude station of the Jungfraujoch (46.5°N, 8°E, 3580 m asl) has indeed allowed to derive column changes ranging from +0.72% in 1987-1988 to +0.14% in 1999-2000 (Zander et al., 2002), relative to 1988 and 2000, respectively. More recently and for the same site, Duchatelet et al. (2010) have even reported a significant slowdown of -0.02%/yr between years 2000 and 2005. This study also showed that since then, CH4 is on the rise again, at a rate close to +0.30%/yr. While the numbers reported here above have been derived from the Fourier Transform Infrared (FTIR) data set starting in 1984, earlier pioneering observations have been collected at the Jungfraujoch since 1950, using grating spectrometers. During the 1958-1975 period, the main objectives has been the study of the solar photosphere in the visible and the near infrared and the publication of high-resolution solar atlases. From 1976 to 1989, narrow-band IR solar absorption observations achieving a spectral resolution of about 0.02 cm-1 have been recorded with the high-performance double-pass grating spectrometer. Analysis of these historical spectra provides a unique opportunity to extend the Jungfraujoch’s total column time series of important atmospheric gases, including methane, by nearly 10 years. The aim of this contribution is to present the inversion strategy adopted to derive CH4 from the grating spectra, using the SFIT-2 algorithm (v3.91) We will evaluate the impact of resolution, spectroscopic parameters (from the EU HYMN project -see www.knmi.nl/samen/hymn-, and from HITRAN 2004), atmospheric pressure and temperature profiles on the error budget. The 1976-1989 total column time series produced will be presented and critically discussed. In particular, we will identify and correct for possible biases between double-pass grating spectrometer measurements and more recent FTIR total columns. The harmonized and consolidated time series will be investigated to characterize the long-term trend of methane for the 1976-2010 time period. Comparisons with synthetic data produced by the CHASER 3-dimensional chemical transport model will also be presented and analyzed. [less ▲]

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See detailTrend evolution and seasonal variation of tropospheric and stratospheric carbonyl sulfide (OCS) above Jungfraujoch
Lejeune, Bernard ULg; Mahieu, Emmanuel ULg; Duchatelet, Pierre ULg et al

in Geophysical Research Abstracts (2011), 13

Carbonyl sulfide (OCS) is the most abundant sulfur-containing trace gas in the atmosphere and accounts for a substantial portion of the sulfur in the stratospheric aerosol layer which influences the ... [more ▼]

Carbonyl sulfide (OCS) is the most abundant sulfur-containing trace gas in the atmosphere and accounts for a substantial portion of the sulfur in the stratospheric aerosol layer which influences the Earth’s radiation budget and stratospheric ozone chemistry. The major identified OCS sources are oceans and anthropogenic emissions, while atmospheric loss and uptake by vegetation and soils constitute the main OCS sinks. The uptake by vegetation strongly influences the distribution and seasonality of OCS throughout most of the Northern Hemisphere, just like for CO2. Montzka et al. (2007) pointed that atmospheric OCS measurements have the potential to constrain the biomass Gross Primary Production (GPP). Unfortunately, there remain large uncertainties on some components strengths of the atmospheric OCS budget. A recent work by Suntharalingam et al. (2008) showed that uptake by plants has been strongly underestimated in actual balanced budgets, suggesting that additional significant OCS sources have still to be identified. In order to improve our understanding of the different processes governing seasonal and inter-annual OCS variability, a new approach has been developed and optimized, using the SFIT-2 algorithm, to retrieve atmospheric abundance of OCS from high-resolution ground-based infrared solar spectra. Our observations are recorded on a regular basis with Fourier Transform Infrared spectrometers (FTIRs), under clear-sky conditions, at the NDACC site (Network for the Detection of Atmospheric Composition Change, http://www.ndacc.org) of the International Scientific Station of the Jungfraujoch (Swiss Alps, 46.5°N, 8.0°E, 3580m asl). Information content analysis of the retrieved OCS products shows us that we are able to distinguish between tropospheric and stratospheric partial column contributions for this species. Thanks to our unique observational database, we have produced an updated OCS long-term trend from 1995 to 2010, representative for both the troposphere and stratosphere at northern mid-latitudes. In this contribution, we will present and critically discuss the recent OCS trend evolution, in particular the end of the slow decline of its abundance observed in 2002 and the maximum reached in 2008. In addition to the OCS inter-annual variations, we will analyze the OCS seasonal cycle during the 15 last years. We will also compare our results with simulations of seasonal OCS variations issued from a 3D global atmospheric chemical transport model (CTM), in order to try to quantify the individual contribution of the various processes playing a role in the Jungfraujoch OCS variability and influencing its atmospheric abundance. [less ▲]

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See detailFirst retrievals of carbon tetrafluoride (CF4) from ground-based FTIR measurements: production and analysis of the two-decadal time series above the Jungfraujoch
Duchatelet, Pierre ULg; Zander, Rodolphe ULg; Mahieu, Emmanuel ULg et al

in Geophysical Research Abstracts (2011)

Carbon tetrafluoride (CF4 or PFC-14) is a potent greenhouse gas that is almost 7400 times more effective (100-yr horizon) than CO2 on a per molecule basis (IPCC, 2007). This high global warming potential ... [more ▼]

Carbon tetrafluoride (CF4 or PFC-14) is a potent greenhouse gas that is almost 7400 times more effective (100-yr horizon) than CO2 on a per molecule basis (IPCC, 2007). This high global warming potential, coming from its medium absorbance combined with a very long atmospheric lifetime (>50000 years; Ravishankara et al., 1993), makes CF4 a key species among the various greenhouse gases targeted by the Kyoto Protocol. In the Northern hemisphere, current atmospheric CF4 concentrations are close to 78 pptv, with a large fraction (around 35 pptv, Mühle et al., 2010) coming from natural processes like lithospheric emissions (Harnisch and Eisenhauer, 1998). In addition, CF4 has been used increasingly since the eighties in electronic and semiconductors industry. The primary aluminum production processes have also been clearly identified as an important anthropogenic source of CF4 emissions. The partitioning between these two main sources is however problematic, principally due to lacking or incomplete CF4 emission factors from inventories performed in industrial fields (e.g. International Aluminum Institute, 2009). Recent in situ ground level measurements of CF4 in the Northern hemisphere (Khalil et al., 2003; Mühle et al., 2010) or remotely from space (Rinsland et al., 2006) have indicated a significant slowdown in the increase rate of atmospheric CF4. This probably results from measures adopted by the aluminum industry aiming at the reduction of the frequency and duration of “anode effects” and therefore of related PFCs emissions (International Aluminum Institute, 2009). The present contribution reports on the long-term evolution (1990-2010) of the atmospheric carbon tetrafluoride total vertical abundance derived from ground-based Fourier transform infrared (FTIR) solar spectroscopy observations around 1285 cm-1 at the Jungfraujoch (46.5°N, 8.0°E, 3580m asl) and compares our findings with results available in the literature. To our knowledge, no equivalent time series (i.e. based on ground-based FTIR technique) has been published to date. [less ▲]

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See detailFirst retrievals of methyl chloride from ground-based high-resolution FTIR solar observations
Mahieu, Emmanuel ULg; Harrison, Jeremy; Bernath, Peter F. et al

in Geophysical Research Abstracts (2011), 13

Methyl chloride (CH3Cl) is one of the most abundant chlorine-bearing gas in the Earth’s troposphere and a significant contributor to the organic chlorine budget. Measurements by in situ networks indicate ... [more ▼]

Methyl chloride (CH3Cl) is one of the most abundant chlorine-bearing gas in the Earth’s troposphere and a significant contributor to the organic chlorine budget. Measurements by in situ networks indicate a mean volume mixing ratio of 550 pptv, with a significant seasonal cycle of about 80 pptv, peak to peak. This species also exhibits inter-annual variability, but no long-term trend. Major sources are from tropical and sub-tropical plants and dead leaves, the oceans and biomass burning. Some industrial processes and waste incineration further add to the emissions. Oxidation by the hydroxyl radical is by far the largest CH3Cl sink, followed by soil uptake. Although balanced, its atmospheric budget is still affected by large uncertainties and contributions from unidentified sources and sinks cannot be ruled out. Methyl chloride has an atmospheric lifetime of 1 year, a global warming potential of 13 (100-yr horizon) and an ozone depleting potential of 0.02. The retrieval of methyl chloride from ground-based infrared (IR) spectra is very challenging. Indeed, numerous interferences by strong water vapor and methane lines complicate the detection of small CH3Cl absorptions, close to 1%, near 3 microns. In addition, and although weak, ethane features contribute to the difficulty, in particular since a significant number of ethane branches were absent until very recently from official HITRAN compilations. Therefore, the scientific literature does not report thus far about any investigations of CH3Cl from ground-based remote sensing observations. In this contribution, we will present first CH3Cl total column retrievals, using the SFIT-2 algorithm (v3.94) and high-resolution Fourier Transform Infrared (FTIR) solar absorption observations recorded with a Bruker 120HR instrument, at the high altitude station of the Jungfraujoch (46.5°N, 8°E, 3580 m asl), within the framework of the Network for the Detection of Atmospheric Composition Change (NDACC, visit http://www.ndacc.org). In our retrievals, we use new ethane absorption cross sections recorded at the Molecular Spectroscopy Facility of the Rutherford Appleton Laboratory (Harrison et al., 2010). They were calibrated in intensity by using reference low-resolution spectra from the Pacific Northwest National Laboratory (PNNL) IR database. These new cross sections were recently released as a HITRAN update (see http://www.hitran.com). Pseudoline parameters fitted to these ethane spectra have been combined with HITRAN 2004 line parameters (including all the 2006 updates) for all other species encompassed in the selected microwindows, including our target CH3Cl. We will evaluate the improvement brought by the new ethane line parameters on the fitting residuals, and characterize the quality, the precision and the reliability of the retrieved product. If successful, a long-term CH3Cl total column time series will be produced using the Jungfraujoch observational database, and we will perform preliminary investigations of the seasonal and inter-annual variations of methyl chloride total columns at northern mid-latitudes. [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 ULg; 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 detailFormic acid above the Jungfraujoch during 1985–2007: observed variability, seasonality, but no long-term background evolution
Zander, Rodolphe ULg; Duchatelet, Pierre ULg; Mahieu, Emmanuel ULg et al

in Atmospheric Chemistry and Physics (2010), 10(20), 10047--10065

This paper reports on daytime total vertical column abundances of formic acid (HCOOH) above the Northern mid-latitude, high altitude Jungfraujoch station (Switzerland; 46.5° N, 8.0° E, 3580 m alt.). The ... [more ▼]

This paper reports on daytime total vertical column abundances of formic acid (HCOOH) above the Northern mid-latitude, high altitude Jungfraujoch station (Switzerland; 46.5° N, 8.0° E, 3580 m alt.). The columns were derived from the analysis of infrared solar observations regularly performed with high spectral resolution Fourier transform spectrometers during over 1500 days between September 1985 and September 2007. The investigation was based on the spectrometric fitting of five spectral intervals, one encompassing the HCOOH ν6 band Q branch at 1105 cm−1, and four additional ones allowing to optimally account for critical temperature-sensitive or time-evolving interferences by other atmospheric gases, in particular HDO, CCl2F2 and CHClF2. The main results derived from the 22 years long database indicate that the free tropospheric burden of HCOOH above the Jungfraujoch undergoes important short-term daytime variability, diurnal and seasonal modulations, inter-annual anomalies, but no significant long-term background change. A major progress in the remote determination of the atmospheric HCOOH columns reported here has resulted from the adoption of new, improved absolute spectral line intensities for the infrared ν6 band of trans-formic acid, resulting in retrieved free tropospheric loadings being about a factor two smaller than if derived with previous spectroscopic parameters. Implications of this significant change with regard to earlier remote measurements of atmospheric formic acid and comparison with relevant Northern mid-latitude findings, both in situ and remote, will be assessed critically. Sparse HCOOH model predictions will also be evoked and assessed with respect to findings reported here. [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 ULg; Demoulin, Philippe ULg; 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 detailLong-term trend of carbon tetrachloride (CCl4) from ground-based high resolution infrared solar spectra recorded at the Jungfraujoch
Rinsland, Curtis P.; Mahieu, Emmanuel ULg; Demoulin, Philippe ULg et al

in Geophysical Research Abstracts (2010), 12(EGU2010-1819-3),

The long-term trend of carbon tetrachloride (CCl4) has been retrieved from infrared high resolution solar absorption spectra encompassing the 1999 to 2010 time period. The measurements were recorded with ... [more ▼]

The long-term trend of carbon tetrachloride (CCl4) has been retrieved from infrared high resolution solar absorption spectra encompassing the 1999 to 2010 time period. The measurements were recorded with a Fourier transform spectrometer at the northern mid-latitude, high altitude Jungfraujoch station in Switzerland (46.5°N latitude, 8.0°E longitude, 3580 m altitude). Total columns were derived from the region of the strong CCl4 _3 band at 794 cm􀀀1 accounting for all interfering molecules (e.g. H2O, O3) with significant improvement in the residuals obtained by also taking into account the line mixing in a nearby CO2 Q branch, a procedure not implemented in previous remote sensing CCl4 retrievals though its importance has been noted in several papers. The time series shows a statistically-significant long-term decrease in the CCl4 total atmospheric burden of -1.18_0.10 %/yr, at the 95% confidence level, using 2005 as reference. Furthermore, fit to the total column data set also reveals a seasonal cycle with a peak-to-peak amplitude of 10.2%, with minimum and maximum values found in mid-February and early August, respectively. This seasonal modulation can however be attributed to tropopause height changes throughout the season. The results quantify the continued impact of the regulations implemented by the Montreal Protocol and its strengthening amendments and adjustments for a molecule with high global warming potential. Although a statistically significant decrease in the total column is inferred, the CCl4 molecule remains an important contributor to the stratospheric chlorine budget and burden. [less ▲]

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