References of "Lejeune, Bernard"
     in
Bookmark and Share    
Full Text
See detailTrend evolution of Carbonyl Sulfide above Jungfraujoch
Lejeune, Bernard ULg

Conference (2014, May 08)

Detailed reference viewed: 14 (3 ULg)
Full Text
Peer Reviewed
See detailLong-term evolution and seasonal modulation above Jungfraujoch (46.5°N, 8.0°E): Optimisation of the retrieval strategy, comparison with model and independant observations
Bader, Whitney ULg; Stavrakou, T; Muller, J-F et al

in Atmospheric Measurement Techniques. Papers in Open Discussion (2014), 7

Methanol (CH3OH) is the second most abundant organic compound in the Earth's atmosphere after methane. In this work, we present the first long-term time series of methanol total, lower tropospheric and ... [more ▼]

Methanol (CH3OH) is the second most abundant organic compound in the Earth's atmosphere after methane. In this work, we present the first long-term time series of methanol total, lower tropospheric and upper tropospheric-lower stratospheric partial columns derived from the analysis of high resolution Fourier transform infrared solar spectra recorded at the Jungfraujoch station (46.5° N, 3580 m a.s.l.). The retrieval of methanol is very challenging due to strong absorptions of ozone in the region of the selected υ8 band of CH3OH. Two wide spectral intervals have been defined and adjusted in order to maximize the information content. Methanol does not exhibit a significant trend over the 1995–2012 time period, but a strong seasonal modulation characterized by maximum values and variability in June–July, minimum columns in winter and a peak-to-peak amplitude of 130%. In situ measurements performed at the Jungfraujoch and ACE-FTS occultations give similar results for the methanol seasonal variation. The total and lower tropospheric columns are also compared with IMAGESv2 model simulations. There is no systematic bias between the observations and IMAGESv2 but the model underestimates the peak-to-peak amplitude of the seasonal modulations. [less ▲]

Detailed reference viewed: 6 (3 ULg)
Full Text
See detailLong-term evolution and seasonal modulation above Jungfraujoch (46.5°N, 8.0°E): Optimisation of the retrieval strategy, comparison with model and independant observations
Bader, Whitney ULg; Stavrakou, J; Muller, J-F et al

Poster (2014, May)

Methanol (CH3OH) is the second most abundant organic compound in the Earth’s atmosphere after methane. In this work, we present the first long-term time series of methanol total, lower tropospheric and ... [more ▼]

Methanol (CH3OH) is the second most abundant organic compound in the Earth’s atmosphere after methane. In this work, we present the first long-term time series of methanol total, lower tropospheric and upper tropospheric-lower stratospheric partial columns derived from the analysis of high resolution Fourier transform infrared solar spectra recorded at the Jungfraujoch station (46.5°N, 3580 m a.s.l.). The retrieval of methanol is very challenging due to strong absorptions of ozone in the region of the selected 8 band of CH3OH. Two wide spectral intervals have been defined and adjusted in order to maximize the information content. Methanol does not exhibit a significant trend over the 1995-2012 time period, but a strong seasonal modulation characterized by maximum values and variability in June-July, minimum columns in winter and a peak-to-peak amplitude of 130 %. In situ measurements performed at the Jungfraujoch and ACE-FTS occultations give similar results for the methanol seasonal variation. The total and lower tropospheric columns are also compared with IMAGESv2 model simulations. There is no systematic bias between the observations and IMAGESv2 but the model underestimates the peak-to-peak amplitude of the seasonal modulations. [less ▲]

Detailed reference viewed: 7 (2 ULg)
Full Text
Peer Reviewed
See detailSpectrometric monitoring of atmospheric carbon tetrafluoride (CF4) above the Jungfraujoch station since 1989: evidence of continued increase but at a slowing rate
Mahieu, Emmanuel ULg; Zander, Rodolphe ULg; Toon, G. C. et al

in Atmospheric Measurement Techniques (2014), 7

The long-term evolution of the vertical column abundance of carbon tetrafluoride (CF4) above the high-altitude Jungfraujoch station (Swiss Alps, 46.5° N, 8.0° E, 3580 m a.s.l.) has been derived from the ... [more ▼]

The long-term evolution of the vertical column abundance of carbon tetrafluoride (CF4) above the high-altitude Jungfraujoch station (Swiss Alps, 46.5° N, 8.0° E, 3580 m a.s.l.) has been derived from the spectrometric analysis of Fourier transform infrared solar spectra recorded at that site between 1989 and 2012. The investigation is based on a multi-microwindow approach, two encompassing pairs of absorption lines belonging to the R-branch of the strong ν3 band of CF4 centered at 1283 cm−1, and two additional ones to optimally account for weak but overlapping HNO3 interferences. The analysis reveals a steady accumulation of the very long-lived CF4 above the Jungfraujoch at mean rates of (1.38 ± 0.11) × 1013 molec cm−2 yr−1 from 1989 to 1997, and (0.98 ± 0.02) × 1013 molec cm−2 yr−1 from 1998 to 2012, which correspond to linear growth rates of 1.71 ± 0.14 and 1.04 ± 0.02% yr−1 respectively referenced to 1989 and 1998. Related global CF4 anthropogenic emissions required to sustain these mean increases correspond to 15.8 ± 1.3 and 11.1 ± 0.2 Gg yr−1 over the above specified time intervals. Findings reported here are compared and discussed with respect to relevant northern mid-latitude results obtained remotely from space and balloons as well as in situ at the ground, including new gas chromatography mass spectrometry measurements performed at the Jungfraujoch since 2010. [less ▲]

Detailed reference viewed: 54 (20 ULg)
Full Text
See detailOverview of the geophysical data derived from long-term FTIR monitoring activities at the Jungfraujoch NDACC site (46.5ºN) and the PYGCHEM project
Mahieu, Emmanuel ULg; Bovy, Benoît ULg; Bader, Whitney ULg et al

Poster (2013, May 07)

We present an overview of the geophysical data deduced from long-term monitoring activities conducted at the Jungfraujoch station by the University of Liège. Typical results and trend investigations are ... [more ▼]

We present an overview of the geophysical data deduced from long-term monitoring activities conducted at the Jungfraujoch station by the University of Liège. Typical results and trend investigations are presented for hydrogen chloride (HCl) and carbonyl sulfide (OCS). We further display and briefly describe time series for new target gases, namely methanol (CH3OH) and HCFC-142b. We also show some preliminary results for ammonia (NH3) and peroxyacetyl nitrate (PAN). Finally, we present the PyGChem project, a Python interface to the GEOS-Chem model currently under development at ULg. [less ▲]

Detailed reference viewed: 75 (28 ULg)
Full Text
See detailEvolution of methanol (CH3OH) above the Jungfraujoch station (46.5°N) : Variability, seasonal modulation and long-term trend.
Bader, Whitney ULg; Mahieu, Emmanuel ULg; Lejeune, Bernard ULg et al

Poster (2013, April 09)

Methanol (CH3OH) is the second most abundant organic compound in the Earth’s atmosphere with concentrations close to a few ppbv, after methane, despite a short lifetime of a few days (Jacob et al., 2005 ... [more ▼]

Methanol (CH3OH) is the second most abundant organic compound in the Earth’s atmosphere with concentrations close to a few ppbv, after methane, despite a short lifetime of a few days (Jacob et al., 2005). Natural sources of CH3OH include plant growth, oceans, decomposition of plant matter, oxidation of methane and other VOCs,. . . while anthropogenic sources are from vehicles, industry,. . . biomass burning completes the emission budget. The main sink is the oxidation by hydroxyl radical, leading to the formation of carbon monoxide (CO) and formaldehyde (H2CO). The retrieval of methanol is very challenging due to the presence of strong absorption of ozone and its isotopologues in addition to water vapour and carbon dioxide in the region of the selected strong nu8 band of CH3OH. First retrievals from satellite observations using the Atmospheric Chemistry Experiment infrared Fourier Transform Spectrometer (ACE-FTS) on board the SCISAT satellite have been performed by Dufour et al. (2007 and references therein) using a spectral interval going from 995.5 to 1008.3 cm-1. In 2009, first retrievals from a ground-based FTS, using spectra recorded at Kitt Peak (31.9°N) and a window going from 992 to 999 cm-1 have been reported by Rinsland et al. (2009), followed by Vigouroux et al. (2012 and references therein) who used yet another spectral interval going from 1029 to 1037cm-1. From those former retrieval strategies and also considering the Mahieu et al. (2012) contribution, we redefined our spectral intervals to maximize the information content. Indeed, our first window, starting from 992 to 1008.3 cm-1, is issued from the merge of Rinsland et al. and Dufour et al. windows while our second, going from 1029 to 1037 cm-1, is the one used by Vigouroux et al.With this new combination of windows, we were able to enlarge the range of zenith angles providing robust results while maintaining good correlation between our two windows; this also resulted in an improvement of the fitting residuals and of the information content. We used the 2008 HITRAN compilation (Rothman et al., 2009) for spectroscopic parameters. However, systematic residuals still remain in the 1033 cm-1 region which are attributed to unsatisfactory line parameters for methanol. New cross sections recorded at the Molecular Spectroscopy Facility of the Rutherford Appleton Laboratory (Harrison et al. 2012) and calibrated in intensity by using the reference spectra from the Pacific Northwest National Laboratory (PNNL) IR database will be tested as soon as converted into pseudolines. In this work, we will present the first long-term time series of methanol total columns, resulting from the implementation of our new retrieval strategy. All retrievals have been performed with the SFIT2 algorithm (v 3.91) (Rinsland et al., 1998) using a series of about 7 000 spectra recorded between 1995 and 2012, with zenith angles between 60 and 85°. These solar absorption observations have been recorded with a high-resolution FTIR 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). [less ▲]

Detailed reference viewed: 55 (21 ULg)
Full Text
See detailFirst retrievals of HCFC-142b from ground-based high resolution FTIR solar observations: application to high altitude Jungfraujoch spectra
Mahieu, Emmanuel ULg; O'Doherty, Simon; Reimann, Stefan et al

in Geophysical Research Abstracts (2013), 15

Hydrofluorocarbons (HCFCs) are the first substitutes to the long-lived ozone depleting halocarbons, in particular the chlorofluorocarbons (CFCs). Given the complete ban of the CFCs by the Montreal ... [more ▼]

Hydrofluorocarbons (HCFCs) are the first substitutes to the long-lived ozone depleting halocarbons, in particular the chlorofluorocarbons (CFCs). Given the complete ban of the CFCs by the Montreal Protocol, its Amendments and Adjustments, HCFCs are on the rise, with current rates of increase substantially larger than at the beginning of the 21st century. HCFC-142b (CH3CClF2) is presently the second most abundant HCFC, after HCFC-22 (CHClF2). It is used in a wide range of applications, including as a blowing foam agent, in refrigeration and air-conditioning. Its concentration will soon reach 25 ppt in the northern hemisphere, with mixing ratios increasing at about 1.1 ppt/yr [Montzka et al., 2011]. The HCFC-142b lifetime is estimated at 18 years. With a global warming potential of 2310 on a 100-yr horizon, this species is also a potent greenhouse gas [Forster et al., 2007]. First space-based retrievals of HCFC-142b have been reported by Dufour et al. [2005]. 17 occultations recorded in 2004 by the Canadian ACE-FTS instrument (Atmospheric Chemistry Experiment – Fourier Transform Spectrometer, onboard SCISAT-1) were analyzed, using two microwindows (1132.5–1135.5 and 1191.5–1195.5 cm-1). In 2009, Rinsland et al. determined the HCFC-142b trend near the tropopause, from the analysis of ACE-FTS observations recorded over the 2004–2008 time period. The spectral region used in this study extended from 903 to 905.5 cm-1. In this contribution, we will present the first HCFC-142b measurements from ground-based high-resolution Fourier Transform Infrared (FTIR) solar spectra. We use observations recorded at the high altitude station of the Jungfraujoch (46.5°N, 8°E, 3580 m asl), with a Bruker 120HR instrument, in the framework of the Network for the Detection of Atmospheric Composition Change (NDACC, visit http://www.ndacc.org). The retrieval of HCFC-142b is very challenging, with simulations indicating only weak absorptions, lower than 1% for low sun spectra and current concentrations. Among the four microwindows tested, the region extending from 900 to 906 cm-1 proved to be the most appropriate, with limited interferences, in particular from water vapor. A total column time series spanning the 2004-2012 time period will be presented, analyzed and critically discussed. After conversion of our total columns to concentrations, we will compare our results with in situ measurements performed in the northern hemisphere by the AGAGE network. [less ▲]

Detailed reference viewed: 71 (18 ULg)
Full Text
Peer Reviewed
See detailGround-based remote sensing of tropospheric water vapour isotopologues within the project MUSICA
Schneider, M.; Barthlott, S.; Hase, F. et al

in Atmospheric Measurement Techniques (2012), 5(2012), 3007-3027

Within the project MUSICA (MUlti-platform remote Sensing of Isotopologues for investigating the Cycle of Atmospheric water), long-term tropospheric water vapour isotopologue data records are provided for ... [more ▼]

Within the project MUSICA (MUlti-platform remote Sensing of Isotopologues for investigating the Cycle of Atmospheric water), long-term tropospheric water vapour isotopologue data records are provided for ten globally distributed ground-based mid-infrared remote sensing stations of the NDACC (Network for the Detection of Atmospheric Composition Change). We present a new method allowing for an extensive and straightforward characterisation of the complex nature of such isotopologue remote sensing datasets. We demonstrate that the MUSICA humidity profiles are representative for most of the troposphere with a vertical resolution ranging from about 2 km (in the lower troposphere) to 8 km (in the upper troposphere) and with an estimated precision of better than 10%. We find that the sensitivity with respect to the isotopologue composition is limited to the lower and middle troposphere, whereby we estimate a precision of about 30‰ for the ratio between the two isotopologues HD16O and H216O. The measurement noise, the applied atmospheric temperature profiles, the uncertainty in the spectral baseline, and the cross-dependence on humidity are the leading error sources. We introduce an a posteriori correction method of the cross-dependence on humidity, and we recommend applying it to isotopologue ratio remote sensing datasets in general. In addition, we present mid-infrared CO2 retrievals and use them for demonstrating the MUSICA network-wide data consistency. In order to indicate the potential of long-term isotopologue remote sensing data if provided with a well-documented quality, we present a climatology and compare it to simulations of an isotope incorporated AGCM (Atmospheric General Circulation Model). We identify differences in the multi-year mean and seasonal cycles that significantly exceed the estimated errors, thereby indicating deficits in the modeled atmospheric water cycle. [less ▲]

Detailed reference viewed: 50 (6 ULg)
Full Text
Peer Reviewed
See detailAnalysis of stratospheric NO2 trends above Jungfraujoch using ground-based UV-visible, FTIR, and satellite nadir observations
Hendrick, F; Mahieu, Emmanuel ULg; Bodeker, G E et al

in Atmospheric Chemistry and Physics (2012), 12

The trend in stratospheric NO2 column at the NDACC (Network for the Detection of Atmospheric Composition Change) station of Jungfraujoch (46.5°N, 8.0°E) is assessed using ground-based FTIR and zenith ... [more ▼]

The trend in stratospheric NO2 column at the NDACC (Network for the Detection of Atmospheric Composition Change) station of Jungfraujoch (46.5°N, 8.0°E) is assessed using ground-based FTIR and zenith-scattered visible sunlight SAOZ measurements over the period 1990 to 2009 as well as a composite satellite nadir data set constructed from ERS-2/GOME, ENVISAT/SCIAMACHY, and METOP-A/GOME-2 observations over the 1996–2009 period. To calculate the trends, a linear least squares regression model including explanatory variables for a linear trend, the mean annual cycle, the quasi-biennial oscillation (QBO), solar activity, and stratospheric aerosol loading is used. For the 1990–2009 period, statistically indistinguishable trends of -3.7±1.1%/decade and -3.6±0.9%/decade are derived for the SAOZ and FTIR NO2 column time series, respectively. SAOZ, FTIR, and satellite nadir data sets show a similar decrease over the 1996–2009 period, with trends of -2.4±1.1%/decade, -4.3±1.4%/decade, and -3.6±2.2%/decade, respectively. The fact that these declines are opposite in sign to the globally observed +2.5%/decade trend in N2O, suggests that factors other than N2O are driving the evolution of stratospheric NO2 at northern mid-latitudes. Possible causes of the decrease in stratospheric NO2 columns have been investigated. The most likely cause is a change in the NO2/NO partitioning in favor of NO, due to a possible stratospheric cooling and a decrease in stratospheric chlorine content, the latter being further confirmed by the negative trend in the ClONO2 column derived from FTIR observations at Jungfraujoch. Decreasing ClO concentrations slows the NO+ ClO -> NO2 + Cl reaction and a stratospheric cooling slows the NO+O3 -> NO2 +O2 reaction, leaving more NOx in the form of NO. The slightly positive trends in ozone estimated from ground- and satellitebased data sets are also consistent with the decrease of NO2 through the NO2 +O3 -> NO3 +O2 reaction. Finally, we cannot rule out the possibility that a strengthening of the Dobson-Brewer circulation, which reduces the time available for N2O photolysis in the stratosphere, could also contribute to the observed decline in stratospheric NO2 above Jungfraujoch. [less ▲]

Detailed reference viewed: 122 (19 ULg)
Full Text
See detailLong-term trends of NO above northern mid-latitudes as inferred from Jungfraujoch, HALOE and ACE-FTS solar observations
Demoulin, Philippe ULg; Mahieu, Emmanuel ULg; Servais, Christian ULg et al

Poster (2012, August 27)

Routine FTIR solar observations are performed by the University of Liège at the Jungfraujoch station (Swiss Alps, 3580 m altitude, NDACC station) since 1985. The analysis of the recorded spectra allows to ... [more ▼]

Routine FTIR solar observations are performed by the University of Liège at the Jungfraujoch station (Swiss Alps, 3580 m altitude, NDACC station) since 1985. The analysis of the recorded spectra allows to derive total and partial columns of more than 20 different atmospheric gases. Among them, gases belonging to the total reactive nitrogen NOy (NO, NO2, HNO3 and ClONO2), to the total inorganic chlorine Cly (HCl and ClONO2) and to the total inorganic fluorine Fy (HF and COF2) families. In this communication, budgets of these gas families are investigated, and their short term, seasonal and inter-annual variations as well as their long-term trends are determined for the time period ranging from the mid-1980s up to the end of 2011. We also investigate the evolution of the same gases, when available, derived from ground-based UV-vis (1990-present) and from HALOE (1991-2004) and ACE-FTS (2004-present) satellite observations. We evaluate the consistency between the trends characterizing these various species, as deduced from the ground- and space-based time series. [less ▲]

Detailed reference viewed: 11 (3 ULg)
Full Text
See detailRetrieval of methanol (CH3OH) above the high-altitude Jungfraujoch station (46.5ºN): preliminary total column time series, long-term trend and seasonal modulation
Mahieu, Emmanuel ULg; Bader, Whitney ULg; Bovy, Benoît ULg et al

Poster (2012, June)

Methanol (CH3OH) is a key organic compound in the Earth’s troposphere, with reported concentrations of the order of a few ppbv. It is indeed the second most abundant organic atmospheric compound after ... [more ▼]

Methanol (CH3OH) is a key organic compound in the Earth’s troposphere, with reported concentrations of the order of a few ppbv. It is indeed the second most abundant organic atmospheric compound after methane. Its lifetime is estimated to a few days. Natural sources of CH3OH include plant growth, oceans, decomposition of plant matter, oxidation of methane,… They are complemented by anthropogenic (from vehicles, industry) and biomass burning emissions. Oxidation by the hydroxyl radical is the main sink, leading to the formation of carbon monoxide (CO) and formaldehyde (H2CO). The first reported retrievals of methanol used a microwindow extending from 992 to 999 cm-1 or from 1029 to 1037 cm-1. In both cases, lines of the strong ν8 band of CH3OH were adjusted, accounting for interferences by several isotopologues of ozone and by water vapor. In this contribution, we present first retrievals of CH3OH from observations recorded at the high-altitude station of the Jungfraujoch (46.5°N, 8°E, 3580 m asl), with a Bruker 120HR spectrometer, in the framework of the Network for the Detection of Atmospheric Composition Change (NDACC, visit http://www.ndacc.org). A strategy maximizing the information content and combining the 992-999 and 1029-1037 cm-1 domains has been set up and used. A preliminary long-term CH3OH total column time series derived from the Jungfraujoch observational database allows us to investigate the seasonal variation and long-term trend of this species at northern mid-latitudes. [less ▲]

Detailed reference viewed: 58 (21 ULg)
Full Text
See detailTrend evolution of carbonyl sulfide above Jungfraujoch deduced from ground-based FTIR and ACE-FTS satellite observations
Lejeune, Bernard ULg

Conference (2012, May 23)

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. There remain large uncertainties on some components strengths of the atmospheric OCS budget and on the OCS contribution for sustaining the Stratospheric Sulfate Aerosol (SSA) layer at background levels during quiet volcanic periods. Monitoring OCS trends can help improving our knowledge about these uncertainties. Using the SFIT-2 algorithm to retrieve atmospheric abundance of OCS from high-resolution ground-based infrared solar spectra recorded on a regular basis with a Fourier Transform Infrared spectrometer (FTIR), 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), we have produced an updated OCS long-term trend from 1995 to 2011, representative for both the troposphere and stratosphere at northern mid-latitudes. In this contribution, we 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. Comparisons with in-situ measurements in a comparable site and with ACE-FTS satellite observations are in good agreement. They confirm the tropospheric nature of the OCS evolution and suggest that OCS is probably not the main contributor of the SSA layer background level. Some potential anthropogenic causes are also discussed, as aluminium production and coal combustion in China. [less ▲]

Detailed reference viewed: 93 (18 ULg)
Full Text
See detailSeeking for the optimum retrieval strategy of methanol (CH3OH) from ground-based high-resolution FTIR solar observations recorded at the high-altitude Jungfraujoch station (46.5ºN)
Mahieu, Emmanuel ULg; Bader, Whitney ULg; Lejeune, Bernard ULg et al

in Geophysical Research Abstracts (2012), 14

Methanol (CH3OH) is a key organic compound in the Earth’s troposphere, with reported concentrations of the order of a few ppbv. It is indeed the second most abundant organic atmospheric compound after ... [more ▼]

Methanol (CH3OH) is a key organic compound in the Earth’s troposphere, with reported concentrations of the order of a few ppbv. It is indeed the second most abundant organic atmospheric compound after methane (Jacob et al., 2005). The same authors have estimated its lifetime to a few days. Natural sources of CH3OH include plant growth, oceans, decomposition of plant matter, oxidation of methane,. . . They are complemented by anthropogenic (from vehicles, industry) and biomass burning emissions. Oxidation by the hydroxyl radical is the main sink, leading to the formation of carbon monoxide (CO) and formaldehyde (H2CO) (Rinsland et al., 2009; Stavrakou et al., 2011, and references therein). The first retrievals of methanol from ground-based Fourier Transform Infrared (FTIR) spectra have been reported by Rinsland et al. (2009), using spectra recorded at Kitt Peak (31.9ºN) and a microwindow extending from 992 to 999 cm-1. Soon after, Stavrakou et al. (2011) used another spectral interval from 1029 to 1037 cm-1, for methanol retrievals at Reunion Island (21ºS). In both cases, lines of the strong nu8 band of CH3OH were adjusted, accounting for interferences by several isotopologues of ozone and by water vapor. In this contribution, we will present first retrievals of CH3OH from observations recorded at the high-altitude station of the Jungfraujoch (46.5ºN, 8ºE, 3580 m asl), with a Bruker 120HR spectrometer, in the framework of the Network for the Detection of Atmospheric Composition Change (NDACC, visit http://www.ndacc.org). We will implement existing retrieval approaches –and possibly additional one(s)– to determine which strategy is the most appropriate for our dry high-altitude site. If successful, a long-term CH3OH total column time series will be produced using the Jungfraujoch observational database, and we will perform preliminary investigations to characterize the seasonal and inter-annual variations of this species at northern mid-latitudes. [less ▲]

Detailed reference viewed: 75 (30 ULg)
Full Text
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 ▲]

Detailed reference viewed: 157 (20 ULg)
Full Text
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 ▲]

Detailed reference viewed: 179 (34 ULg)
Full Text
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 ▲]

Detailed reference viewed: 8 (2 ULg)
Full Text
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 ▲]

Detailed reference viewed: 97 (20 ULg)
Full Text
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 ▲]

Detailed reference viewed: 291 (43 ULg)
Full Text
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 ▲]

Detailed reference viewed: 75 (18 ULg)