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See detailOzone tropospheric and stratospheric trends (1995-2012) at six ground-based FTIR stations (28°N to 79°N)
Vigouroux, Corinne; De Mazière, Martine; Demoulin, Philippe ULg et al

Poster (2013, April)

In the frame of the Network for the Detection of Atmospheric Composition Change (NDACC), contributing ground-based stations have joined their efforts to homogenize and optimize the retrievals of ozone ... [more ▼]

In the frame of the Network for the Detection of Atmospheric Composition Change (NDACC), contributing ground-based stations 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. In a previous study, Vigouroux et al. (2008) applied a bootstrap resampling method to determine the trends of the ozone total and four partial columns, over the period 1995-2004 at Western European stations. The updated trends for the period 1995-2009 have been published in the WMO 2010 report. Here, we present the updated trends and their uncertainties, for the 1995-2012 period, for the different altitude ranges, above five European stations (28°N-79°N) and above the station Thule, Greenland (77°N). In this work, the trends have been estimated using a multiple regression model including some explanatory variables responsible for the ozone variability, such as the Quasi Biennial Oscillation (QBO), the solar flux, the Arctic Oscillation (AO) or El Niño-Southern Oscillation (ENSO). A major result is the significant positive trend of ozone in the upper stratosphere, observed at the Jungfraujoch (47°N), which is a typical mid-latitude site, as well as at the high latitude stations. This positive trend in the upper stratosphere at Jungfraujoch provides a sign of ozone recovery at mid-latitudes. [less ▲]

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See detailFourier Transform Infrared Spectrometry
Schneider, Matthias; Demoulin, Philippe ULg; Sussmann, Ralf et al

in Kämpfer, Niklaus (Ed.) Monitoring Atmospheric Water Vapour : Ground-Based Remote Sensing and In-situ Methods (2012)

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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 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 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 detailObserved and simulated time evolution of HCl, ClONO2, and HF total column abundances
Kohlhepp, R.; Ruhnke, R.; Chipperfield, M. P. et al

in Atmospheric Chemistry & Physics Discussions (2011), 11(12), 32085--32160

Time series of total column abundances of hydrogen chloride (HCl), chlorine nitrate (ClONO2), and hydrogen fluoride (HF) were determined from ground-based Fourier transform infrared (FTIR) spectra ... [more ▼]

Time series of total column abundances of hydrogen chloride (HCl), chlorine nitrate (ClONO2), and hydrogen fluoride (HF) were determined from ground-based Fourier transform infrared (FTIR) spectra recorded at 17 sites belonging to the Network for the Detection of Atmospheric Composition Change (NDACC) and located between 80.05° N and 77.82° S. These measurements are compared with calculations from five different models: the two-dimensional Bremen model, the two chemistry-transport models KASIMA and SLIMCAT, and the two chemistry-climate models EMAC and SOCOL. The overall agreement between the measurements and models for the total column abundances and the seasonal cycles is good. Trends of HCl, ClONO2, and HF are calculated from both measurement and model time series data, with a focus on the time range 2000–2009. Their precision is estimated with the bootstrap resampling method. The sensitivity of the trend results with respect to the fitting function, the time of year chosen and time series length is investigated, as well as a bias due to the irregular sampling of the measurements. For the two chlorine species, a decrease is expected during this period because the emission of their prominent anthropogenic source gases (solvents, chlorofluorocarbons (CFCs)) was restricted by the Montreal Protocol 1987 and its amendments and adjustments. As most of the restricted source gases also contain fluorine, the HF total column abundance was also influenced by the above-mentioned regulations in the time period considered. The measurements and model results investigated here agree qualitatively on a decrease of the chlorine species by around −1 % yr−1. The models simulate an increase of HF of around +1 % yr−1. This also agrees well with most of the measurements, but some of the FTIR series in the Northern Hemisphere show a stabilisation or even a decrease in the last few years. In general, for all three gases, the measured trends vary more strongly with latitude and hemisphere than the modelled trends. Relative to the FTIR measurements, the models tend to underestimate the decreasing chlorine trends and to overestimate the fluorine increase in the Northern Hemisphere. At most sites, the models simulate a stronger decrease of ClONO2 than of HCl. In the FTIR measurements, this difference between the trends of HCl and ClONO2 depends strongly on latitude, especially in the Northern Hemisphere. [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 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 detailMeasured and modelled trends of stratopsheric Cly and Fy column amounts in the northern hemisphere
Ruhnke, Roland; Blumenstock, Thomas; Duchatelet, Pierre ULg et al

Poster (2007, April)

Reactive inorganic chlorine plays a crucial role in the stratospheric ozone depletion. To stabilize and enable a recovering of the stratospheric ozone layer, the Montreal protocol and its amendments and ... [more ▼]

Reactive inorganic chlorine plays a crucial role in the stratospheric ozone depletion. To stabilize and enable a recovering of the stratospheric ozone layer, the Montreal protocol and its amendments and adjustments have been progressively implemented to reduce or even stop the production and emission of important chlorinated source gases (CFCs, HCFCs, CCl4, CH3CCl3, and Halons). As these source gases are photolysed in the stratosphere into inorganic chlorine and fluorine, respectively, the turn over of the inorganic chlorine (HCl and ClONO2) and slowing down of fluorine (HF and COF2) reservoirs act as a verification of the effectiveness of these protocols. Here we present results of long-term measurements of the stratospheric column of HCl, ClONO2, and HF obtained at different stations in the northern hemisphere (Ny Alesund, Kiruna, Zugspitze, Jungfraujoch, Izana, all affiliated to the NDACC, Network for the Detection of Atmospheric Composition Change) within the PEP (Pole- Equator-Pole) network. These time series are interpreted with model calculations performed with a state of the art 2-D model and the 3-D CTM KASIMA with respect to the determination of the slowing down or turn over, respectively. In addition, trend parameters calculated using different approaches (e.g. linear trend, bootstrap-method) will be presented and intercompared. [less ▲]

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

in Atmospheric Chemistry and Physics (2007), 7

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

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

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See detailOn the line parameters for the X 1sigma+g (1–0) infrared quadrupolar transitions of 14N2
Goldman, Aaron; Tipping, R.H.; Ma, Q. et al

in Journal of Quantitative Spectroscopy & Radiative Transfer (2007), 103

Re-examination of the 14N2 X 1sigma+g (1–0) line parameters in the HITRAN database showed that the vibration–rotation interaction effect on the line intensities has been neglected, and that the halfwidths ... [more ▼]

Re-examination of the 14N2 X 1sigma+g (1–0) line parameters in the HITRAN database showed that the vibration–rotation interaction effect on the line intensities has been neglected, and that the halfwidths are not compatible with experimental and theoretical studies. New line parameters have been generated, which improve the consistency and accuracy in individual N2 line retrievals from atmospheric spectra. Unresolved line shape issues require further studies. [less ▲]

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See detailIncreased Northern Hemispheric carbon monoxide burden in the troposphere in 2002 and 2003 detected from the ground and from space
Yurganov, Leonid N.; Duchatelet, Pierre ULg; Dzhola, A. V. et al

in Atmospheric Chemistry and Physics (2005), 5

Carbon monoxide total column amounts in the atmosphere have been measured in the High Northern Hemisphere (30degrees - 90degrees N, HNH) between January 2002 and December 2003 using infrared spectrometers ... [more ▼]

Carbon monoxide total column amounts in the atmosphere have been measured in the High Northern Hemisphere (30degrees - 90degrees N, HNH) between January 2002 and December 2003 using infrared spectrometers of high and moderate resolution and the Sun as a light source. They were compared to ground-level CO mixing ratios and to total column amounts measured from space by the Terra/MOPITT instrument. All these data reveal increased CO abundances in 2002 - 2003 in comparison to the unperturbed 2000 - 2001 period. Maximum anomalies were observed in September 2002 and August 2003. Using a simple two-box model, the corresponding annual CO emission anomalies (referenced to 2000 - 2001 period) have been found equal to 95 Tg in 2002 and 130 Tg in 2003, thus close to those for 1996 and 1998. A good correlation with hot spots detected by a satellite radiometer allows one to assume strong boreal forest fires, occurred mainly in Russia, as a source of the increased CO burdens. [less ▲]

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