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See detailComparison of ground-based remote sensing and in-situ observations of CO, CH4 and O3, accounting for representativeness uncertainty
Henne, S.; Steinbacher, M.; Mahieu, Emmanuel ULg et al

Conference (2013, April)

The EC project NORS (Demonstration Network Of ground-based Remote Sensing Observations in support of the GMES Atmospheric Service) aims at demonstrating the value of ground-based remote sensing data for ... [more ▼]

The EC project NORS (Demonstration Network Of ground-based Remote Sensing Observations in support of the GMES Atmospheric Service) aims at demonstrating the value of ground-based remote sensing data for quality assessment and improvement of the GMES products. As part of NORS CO, CH4, O3 and NO2 tropospheric products as obtained by ground-based remote sensing within the Network for the Detection of Atmospheric Composition Change (NDACC) are compared to continuous surface in-situ measurements that are reported on common international reference scales within the Global Atmospheric Watch (GAW) Programme. However, a direct comparison between the different methods is hindered by different sampling volumes, introducing uncertainties due to representativeness. Here we present a novel method that utilises high-resolution, backward Lagrangian particle dispersion modelling to characterise the transport history of different sampling volumes. Sampling volumes are defined as infinitesimally small point volumes for the in-situ observations and as separate profile segments with horizontal and vertical extent for the remote sensing observations. The characterisation is then used (a) to filter times for which a direct comparison between in-situ and remote sensing data is unfavourable (large representativeness uncertainty) and (b) to construct vertical profiles from the in-situ observations, taking additional information from large scale atmospheric composition models into account. These so called “in-situ” profiles are supposed to be more comparable to the remote sensing profile as the surface value itself, while conserving the high accuracy information of the latter and projecting it onto the profile. Therefore, these profiles allow for a more direct comparison and validation of the remotely sensed profiles. The technique was first applied at two of the four NORS demonstration sites (Jungfraujoch, Switzerland and Izana, Spain) and to the comparison of remote sensing Fourier-transform infrared spectrometer (FTIR) measurements of CO, CH4, and O3 with the responding in-situ observations. While previous studies generally showed good agreement between the two kinds of observation, considerable amounts of scatter were evident. Selecting only situations with relatively small representativeness uncertainty reduces this scatter. Folding the “in-situ” profiles with the averaging kernels of the FTIR retrieval gives a more realistic comparison result that is not influenced by any a-priori assumptions. Results are also discussed with respect to season, time of day and weather type. [less ▲]

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See detailRecent trend anomaly of hydrogen chloride (HCl) at northern mid-latitudes derived from Jungfraujoch, HALOE and ACE-FTS Infrared solar observations
Mahieu, Emmanuel ULg; Zander, Rodolphe ULg; Bernath, Peter F. et al

in Bernath, Peter F. (Ed.) The Atmospheric Chemistry Experiment ACE at 10: A Solar Occultation Anthology (2013)

In this contribution, we analyze infrared solar observations recorded from the ground at the Jungfraujoch station and from space with the HALOE and the ACE-FTS instruments to derive time series of ... [more ▼]

In this contribution, we analyze infrared solar observations recorded from the ground at the Jungfraujoch station and from space with the HALOE and the ACE-FTS instruments to derive time series of stratospheric columns of hydrogen chloride (HCl) at Northern mid-latitudes. We investigate the Jungfraujoch and the composite satellite time series to characterize the evolution of HCl over the last 15 years, i.e. after its peak loading which occurred in 1996 in this region of the Earth’s atmosphere. Trends derived from both data sets are compared and possible causes for the recent change in the stratospheric HCl buildup are evoked. [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 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 detailAssessing the losses of HCFC-22 using ACE-FTS measurements
Kolonjari, F.; Walker, K.A.; Boone, C.D. et al

Scientific conference (2012, November 09)

The annual springtime minimum in stratospheric ozone over the Antarctic is primarily caused by catalytic reactions of ozone and chlorine. The Montreal Protocol on Substances that Deplete the Ozone Layer ... [more ▼]

The annual springtime minimum in stratospheric ozone over the Antarctic is primarily caused by catalytic reactions of ozone and chlorine. The Montreal Protocol on Substances that Deplete the Ozone Layer (with its subsequent amendments) restricts the emissions of ozone depleting substances. HCFC-22 has been the primary replacement for both CFC-11 and CFC-12, which has led to an increase in its atmospheric abundance. The Atmospheric Chemistry Experiment (ACE) is a mission on-board the Canadian satellite SCISAT. The primary instrument on SCISAT is a highresolution infrared Fourier Transform Spectrometer (ACE-FTS). With its wide spectral range, the ACE-FTS is capable of measuring an extensive range of gases including key CFC and HCFC species. The altitude distribution from the ACE-FTS profiles provides information that is complementary to the ground-based measurements that have been used to monitor these species. The ACE-FTS measurements compare well with surface in situ and balloon measurements. A preliminary validation of HCFC-22 using ground-based FTSs is discussed. The zonal mean distribution of HCFC-22 as observed by ACE-FTS is presented. The global distributions of HCFC-22 have been compared to the Global Modelling Initiative (GMI) Combined Stratospheric-Tropospheric Model, a chemistry and transport model. Large differences between the model and ACE-FTS measurements of HCFC-22 reveal issues with the boundary value mixing ratios. The comparison of stratospheric measurements with GMI suggest that there may be a missing loss process in the stratosphere, some issues with transport circulation and polar cap averaging in the current run, or a combination of the two processes. We propose the reaction of HCFC-22 with atomic chlorine as a potentially important loss process in the lowermost stratosphere and the lower stratosphere. [less ▲]

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See detailPost-peak trend in inorganic chlorine (Cly) from Jungfraujoch, ACE-FTS and HALOE infrared solar observations
Mahieu, Emmanuel ULg

Conference (2012, October 17)

Rencent trend in inorganic chlorine are derived from ground-based and satellite occultation measurements performed in the infrared at Northern mid-latitudes. The consistent slowing down in the rate of ... [more ▼]

Rencent trend in inorganic chlorine are derived from ground-based and satellite occultation measurements performed in the infrared at Northern mid-latitudes. The consistent slowing down in the rate of decrease of hydrogen chloride (HCl) and inorganic chlorine (Cly) is presented and possible causes are discussed. [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 detailNORS: Demonstration Network Of ground-based Remote Sensing observations in support of the GMES atmospheric service
De Mazière, M; Hocke, K; Richter, A et al

Poster (2012, September 17)

NORS (Demonstration Network Of ground-based Remote Sensing Observations in support of the GMES Atmospheric Service) aims at demonstrating the value of ground – based remote sensing data from the Network ... [more ▼]

NORS (Demonstration Network Of ground-based Remote Sensing Observations in support of the GMES Atmospheric Service) aims at demonstrating the value of ground – based remote sensing data from the Network for the Detection of Atmospheric Composition Change for quality assessment and improvement of the GMES Atmospheric Service products. [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 detailValidation of ACE-FTS using ground-based FTIR measurements of CFC-11, CFC-12 and HCFC-22
Kolonjari, F.; Mahieu, Emmanuel ULg; Walker, K.A. et al

Poster (2012, July 24)

Satellite data can be an effective global monitoring tool for long-lived compounds in the atmosphere. The Atmospheric Chemistry Experiment (ACE) is a mission on-board the Canadian satellite SCISAT. The ... [more ▼]

Satellite data can be an effective global monitoring tool for long-lived compounds in the atmosphere. The Atmospheric Chemistry Experiment (ACE) is a mission on-board the Canadian satellite SCISAT. The primary instrument on SCISAT is a high-resolution infrared Fourier Transform Spectrometer (ACE-FTS) which is capable of measuring a wide range of gases including key chlorofluorocarbon (CFC) and hydrochlorofluorocarbon (HCFC) species. These families of species are of interest because of their significant contribution to anthropogenic ozone depletion and to global warming. To assess the quality of data derived from satellite measurements, validation using other data sources is critical. Ground-based Fourier transform infrared spectrometers (FTIRs) are particularly useful for this purpose. In this study, five FTIRs located at four sites around the world are used to validate the CFC- 11, CFC-12, and HCFC-22 data products from ACE-FTS. These species are related; HCFC-22 was the primary replacement for CFC-11 and CFC-12 in refrigerant and propellant applications. The five FTIR instruments used in this study record solar absorption spectra at Eureka, Canada, Jungfraujoch, Switzerland, Poker Flat, USA, and Toronto, Canada. Details on the instrumentation at each site will be provided. The retrieval of CFC-11, CFC-12, and HCFC-22 are not standard products for many of these FTIRs, and as such, the initial stage of this study is to develop the retrieval of each species. Harmonization of retrieval parameters between the sites is an important step in this process. The development of these retrievals and preliminary results will be presented. Additionally, a new method for the validation of ACE-FTS measurements will be discussed. [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 detailMeasurements of HCFC-22 and validation update
Kolonjari, F.; Walker, K.A.; Mahieu, Emmanuel ULg et al

Scientific conference (2012, May 24)

This talk reports about global HCFC-22 measurements derived from ACE-FTS occultation observations recorded from 2004 onwards. It further provides information on the validation of ACE-FTS products for CFC ... [more ▼]

This talk reports about global HCFC-22 measurements derived from ACE-FTS occultation observations recorded from 2004 onwards. It further provides information on the validation of ACE-FTS products for CFC-11, -12 and HCFC-22 with ground-based FTIR instruments operated at four sites: Eureka, Poker Flat, Toronto and Jungfraujoch. [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 detailProcess-evaluation of tropospheric humidity simulated by general circulation models using water vapor isotopologues: 1. Comparison between models and observations
Risi, C; Noone, D; Worden, J et al

in Journal of Geophysical Research (2012), 117(D5), 05303

N2 - The goal of this study is to determine how H2O and HDO measurements in water vapor can be used to detect and diagnose biases in the representation of processes controlling tropospheric humidity in ... [more ▼]

N2 - The goal of this study is to determine how H2O and HDO measurements in water vapor can be used to detect and diagnose biases in the representation of processes controlling tropospheric humidity in atmospheric general circulation models (GCMs). We analyze a large number of isotopic data sets (four satellite, sixteen ground-based remote-sensing, five surface in situ and three aircraft data sets) that are sensitive to different altitudes throughout the free troposphere. Despite significant differences between data sets, we identify some observed HDO/H2O characteristics that are robust across data sets and that can be used to evaluate models. We evaluate the isotopic GCM LMDZ, accounting for the effects of spatiotemporal sampling and instrument sensitivity. We find that LMDZ reproduces the spatial patterns in the lower and mid troposphere remarkably well. However, it underestimates the amplitude of seasonal variations in isotopic composition at all levels in the subtropics and in midlatitudes, and this bias is consistent across all data sets. LMDZ also underestimates the observed meridional isotopic gradient and the contrast between dry and convective tropical regions compared to satellite data sets. Comparison with six other isotope-enabled GCMs from the SWING2 project shows that biases exhibited by LMDZ are common to all models. The SWING2 GCMs show a very large spread in isotopic behavior that is not obviously related to that of humidity, suggesting water vapor isotopic measurements could be used to expose model shortcomings. In a companion paper, the isotopic differences between models are interpreted in terms of biases in the representation of processes controlling humidity. [less ▲]

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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 ▲]

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