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(author:Demoulin, Philippe)OR(U012635)

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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 ▲]

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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 ▲]

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See detailTumor microenvironment converts plasmacytoid dendritic cells into immunosuppressive/tolerogenic cells: insight into the molecular mechanisms
Demoulin, Stéphanie ULg; Herfs, Michael ULg; Hubert, Pascale ULg et al

in Journal of Leukocyte Biology (2013), 93

Human pDCs represent a rare population of circulating cells characterized by a rapid and massive TLR-dependent secretion of type I IFN in response to pathogenic agents or danger signals. Through their ... [more ▼]

Human pDCs represent a rare population of circulating cells characterized by a rapid and massive TLR-dependent secretion of type I IFN in response to pathogenic agents or danger signals. Through their capacity to bring together innate and adaptive immunity and to secrete soluble factors controlling cancer development, these cells could represent important actors in antitumor immunity. However, accumulating evidence suggests that pDCs recruited to the tumor microenvironment often display a nonactivated state and are associated with the development and maintenance of immunosuppression. Here, we present an overview of neoplastic lesions associated with an infiltration of immunosuppressive/ tolerogenic pDC. Moreover, as the proper response of pDC against cancer depends on a critical balance between immune-activating and immune-suppressing mechanisms, we summarize current knowledge about the molecular pathways developed by tumors to prevent antitumoral pDC immune responses. A better understanding of the mechanisms regulating pDC function in tumors could aid in the development of new therapies. Indeed, effective cancer vaccines or therapies could combine immunoactivating strategies (i.e., TLR agonists) with elimination of immune-suppressing mechanisms, leading to pDC reprogramming and thus, allowing tumor rejection in a clinical setting. [less ▲]

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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 ▲]

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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 ▲]

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See detailValidation of IASI FORLI carbon monoxide retrievals using FTIR data from NDACC
Kerzenmacher, T; Dils, B; Kumps, N et al

in Atmospheric Measurement Techniques (2012), 5

Carbon monoxide (CO) is retrieved daily and globally from space-borne IASI radiance spectra using the Fast Optimal Retrievals on Layers for IASI (FORLI) software developed at the Université Libre de ... [more ▼]

Carbon monoxide (CO) is retrieved daily and globally from space-borne IASI radiance spectra using the Fast Optimal Retrievals on Layers for IASI (FORLI) software developed at the Université Libre de Bruxelles (ULB). The IASI CO total column product for 2008 from the most recent FORLI retrieval version (20100815) is evaluated using correlative CO profile products retrieved from groundbased solar absorption Fourier transform infrared (FTIR) observations at the following FTIR spectrometer sites from the Network for the Detection of Atmospheric Composition Change (NDACC): Ny-Alesund, Kiruna, Bremen, Jungfraujoch, Izana and Wollongong. In order to have good statistics for the comparisons, we included all IASI data from the same day, within a 100 km radius around the ground-based stations. The individual ground-based data were adjusted to the lowest altitude of the co-located IASI CO profiles. To account for the different vertical resolutions and sensitivities of the ground-based and satellite measurements, the averaging kernels associated with the various retrieved products have been used to properly smooth coincident data products. It has been found that the IASI CO total column products compare well on average with the co-located ground-based FTIR total columns at the selected NDACC sites and that there is no significant bias for the mean values at all stations. [less ▲]

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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 ▲]

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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 ▲]

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See detailFirst steps of a new methodology for integrating ground-based ozone profile data
Pastel, M.; Godin-Beekmann, S.; Mahieu, Emmanuel ULg et al

Poster (2012, August)

A new methodology is developed for integrating complementary ground-based data sources to provide consistent ozone vertical distribution time series as well as tropospheric and stratospheric ozone partial ... [more ▼]

A new methodology is developed for integrating complementary ground-based data sources to provide consistent ozone vertical distribution time series as well as tropospheric and stratospheric ozone partial columns. Primary results are presented for the Alpine station of the Network for the Detection of Atmospheric Composition Changes (NDACC). Ozone measurements from the lidar at Haute-Provence Observatory, the microwave spectrometer at Bern and the FTIR spectrometer at the Jungfrauch station are used for this purpose. First step is to evaluate the validity domain of ozone profile data considered here by assessing instrumental error and vertical resolution. Each instrument has its own vertical resolution; therefore adjustments need to be done for the creation of an homogeneous data set. Indeed, because of the higher resolution of lidar measurements, smoothing of the data is necessary for the comparison with FTIR and microwave measurements. However, smoothing the data induces a loss of scientific information. Therefore a compromise has to be established and discussed. The various intercomparisons provide an evaluation of the differences due to instrumental error and atmospheric variability. The statistical method used for combining the different measurements in order to obtain ozone vertical profile time series consistent with total ozone measurements is then discussed. [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

Poster (2012, August)

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. The retrieval of ethane from ground-based infrared spectra is challenging. Indeed, ethane has a complicated spectrum with many interacting vibrational modes and the current state of ethane parameters in HITRAN (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. 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. We evaluated the impact on spectral residuals induced by the update of two O3 lines (encompassed in the PQ3 µ-window) corrected by P. Chelin (LPMA, Paris, France). We also quantified the improvement brought by the update of the line positions and intensities of methyl chloride (CH3Cl) in the 3.4 µm region (Bray et al., 2011). The ethane a priori volume mixing ratio (VMR) profile and associated covariance are based on synthetic data from CHASER 3-D chemical transport model (CTM). In this contribution, we will present updated ethane (total) 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). Comparisons with synthetic data produced by two chemical transport models (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 detailRetrievals of ethane from groundbased highresolution 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

Scientific conference (2012, June 01)

Ethane (C2H6) is the most abundant Non-Methane HydroCarbon (NMHC) in the Earth’s atmosphere, with a lifetime of approximately 2 months. Its main sources are biomass burning, natural gas loss and biofuel ... [more ▼]

Ethane (C2H6) is the most abundant Non-Methane HydroCarbon (NMHC) in the Earth’s atmosphere, with a lifetime of approximately 2 months. Its main sources are biomass burning, natural gas loss and biofuel consumption. Oxidation by the hydroxyl radical is the major C2H6 sink as it controls its strong modulation throug the year. C2H6 is involved in the formation of tropospheric O3 and in the destruction of atmospheric methane through changes in OH. C2H6 is an indirect greenhouse gas with a net-global warming potential of 5.5 (100-yr horizon). Updates of retrieval parameters such as the spectroscopic linelists have been recently published. We will therefore characterize three µ-windows encompassing the strongest C2H6 features after careful selection of these new parameters, accounting at best for all interfering species. The aim is to lessen the fitting residuals while maximizing the information content, the precision and the reliability of the retrieved product. We will present updated C2H6 total and tropospheric column time series, using the SFIT-2 algorithm (v3.91) and high-resolution Fourier Transform Infrared (FTIR) solar absorption spectra recorded with a Bruker 120HR instrument, at the high altitude research station of the Jungfraujoch (46.5°N, 8.0°E, 3580 m asl), within the framework of the Network for the Detection of Atmospheric Composition Change (NDACC, http://www.ndacc.org). Comparisons with synthetic data produced by chemical transport models will also be presented. [less ▲]

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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 ▲]

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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 and Physics (2012), 12(7), 3527--3556

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. By providing such a near-global overview on ground-based measurements of the two major stratospheric chlorine reservoir species, HCl and ClONO2, the present study is able to confirm the decrease of the atmospheric inorganic chlorine abundance during the last few years. This decrease is expected following the 1987 Montreal Protocol and its amendments and adjustments, where restrictions and a subsequent phase-out of the prominent anthropogenic chlorine source gases (solvents, chlorofluorocarbons) were agreed upon to enable a stabilisation and recovery of the stratospheric ozone layer. The atmospheric fluorine content is expected to be influenced by the Montreal Protocol, too, because most of the banned anthropogenic gases also represent important fluorine sources. But many of the substitutes to the banned gases also contain fluorine so that the HF total column abundance is expected to have continued to increase during the last few years. The 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. Thereby, the ability of the models to reproduce the absolute total column amounts, the seasonal cycles, and the temporal evolution found in the FTIR measurements is investigated and inter-compared. This is especially interesting because the models have different architectures. The overall agreement between the measurements and models for the total column abundances and the seasonal cycles is good. Linear 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. This period is chosen because from most of the measurement sites taking part in this study, data are available during these years. The precision of the trends 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. 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 detailEchecs
Demoulin, Laurent ULg

E-print/Working paper (2012)

Echecs est un roman inédit de Jean-Philippe Toussaint, antérieur à La Salle de bain. Il est ici édité avec un apparat critique: variantes et notes critiques.

Detailed reference viewed: 9 (1 ULg)