References of "Mahieu, Emmanuel"
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See detailRetrievals of formaldehyde from ground-based FTIR and MAX-DOAS observations at the Jungfraujoch station and comparisons with GEOS-Chem and IMAGES model simulations
Franco, Bruno ULg; Hendrick, François; Van Roozendael, Michel et al

Conference (2014, November 07)

As a ubiquitous product of the oxidation of many Volatile Organic Compounds (VOCs), formaldehyde (HCHO) plays a key role as a short-lived and reactive intermediate in the atmospheric photo-oxidation ... [more ▼]

As a ubiquitous product of the oxidation of many Volatile Organic Compounds (VOCs), formaldehyde (HCHO) plays a key role as a short-lived and reactive intermediate in the atmospheric photo-oxidation pathways leading to the formation of tropospheric ozone and secondary organic aerosols. We have successfully retrieved HCHO columns from ground-based Fourier Transform Infrared (FTIR) solar spectra and UV-Visible Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) scans recorded during the July 2010 – December 2012 time period at the Jungfraujoch station (Swiss Alps, 46.5 °N, 8.0 °E, 3580 m a.s.l.). Characterization of the retrieved products has revealed different vertical sensitivity between both remote sensing techniques. Furthermore, HCHO amounts simulated by two state-of-the-art Chemical Transport Models (CTMs), GEOS-Chem and IMAGESv2, have been compared to FTIR total columns and MAX-DOAS 3.6 – 8 km partial columns, accounting for the respective vertical resolution of each ground-based instrument. Using the CTMs outputs as intermediate, FTIR and MAX-DOAS retrievals have shown consistent seasonal modulations of HCHO throughout the investigated period, characterized by summertime maximum and wintertime minimum. Such comparisons have also highlighted that FTIR and MAX-DOAS provide complementary products for HCHO above the Jungfraujoch station. [less ▲]

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See detailRecent Northern Hemisphere stratospheric HCl increase due to atmospheric circulation changes
Mahieu, Emmanuel ULg; Chipperfield, M. P.; Notholt, J. et al

in Nature (2014), 515(7525), 104--107

The abundance of chlorine in the Earth’s atmosphere increased considerably during the 1970s to 1990s, following large emissions of anthropogenic long-lived chlorine-containing source gases, notably the ... [more ▼]

The abundance of chlorine in the Earth’s atmosphere increased considerably during the 1970s to 1990s, following large emissions of anthropogenic long-lived chlorine-containing source gases, notably the chlorofluorocarbons. The chemical inertness of chlorofluorocarbons allows their transport and mixing throughout the troposphere on a global scale[1], before they reach the stratosphere where they release chlorine atoms that cause ozone depletion[2]. The large ozone loss over Antarctica[3] was the key observation that stimulated the definition and signing in 1987 of the Montreal Protocol, an international treaty establishing a schedule to reduce the production of the major chlorine- and bromine-containing halocarbons. Owing to its implementation, the near-surface total chlorine concentration showed a maximum in 1993, followed by a decrease of half a per cent to one per cent per year[4], in line with expectations. Remote-sensing data have revealed a peak in stratospheric chlorine after 1996[5], then a decrease of close to one per cent per year[6,7], in agreement with the surface observations of the chlorine source gases and model calculations[7]. Here we present ground-based and satellite data that show a recent and significant increase, at the 2σ level, in hydrogen chloride (HCl), the main stratospheric chlorine reservoir, starting around 2007 in the lower stratosphere of the Northern Hemisphere, in contrast with the ongoing monotonic decrease of near-surface source gases. Using model simulations, we attribute this trend anomaly to a slowdown in the Northern Hemisphere atmospheric circulation, occurring over several consecutive years, transporting more aged air to the lower stratosphere, and characterized by a larger relative conversion of source gases to HCl. This short-term dynamical variability will also affect other stratospheric tracers and needs to be accounted for when studying the evolution of the stratospheric ozone layer. [less ▲]

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See detailIncrease in northern hemisphere stratospheric hydrogen chloride over recent years
Mahieu, Emmanuel ULg; Chipperfield, MP; Notholt, J et al

Poster (2014, October 07)

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See detailSELF BROADENING COEFFICIENTS AND IMPROVED LINE INTENSITIES FOR THE v7 BAND OF C2H4 NEAR 10.5 µm, AND IMPACT ON ETHYLENE RETRIEVALS FROM JUNGFRAUJOCH SOLAR SPECTRA
Vander Auwera, Jean; Fayt, André; Tudorie, Marcella et al

Poster (2014, September)

Relying on high-resolution Fourier transform infrared (FTIR) spectra, the present work involved extensive measurements of individual line intensities and self-broadening coefficients for the ν7 band of ... [more ▼]

Relying on high-resolution Fourier transform infrared (FTIR) spectra, the present work involved extensive measurements of individual line intensities and self-broadening coefficients for the ν7 band of 12C2H4. The measured self-broadening coefficients exhibit a dependence on both J and Ka. Compared to the corresponding information available in the latest edition of the HITRAN spectroscopic database, the measured line intensities were found to be higher by about 10 % for high J lines in the P branch and lower by about 5 % for high J lines of the R branch, varying between these two limits roughly linearly with the line positions. The impact of the presently measured line intensities on retrievals of atmospheric ethylene in the 949.0–952.0cm 1 microwindow was evaluated using a subset of ground-based high-resolution FTIR solar spectra recorded at the Jungfraujoch station. The use of HITRAN 2012 with line intensities modified to match the present measurements led to a systematic reduction of the measured total columns of ethylene by -4.1 +/- 0.1 %. [less ▲]

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See detailSelf-broadening coefficients and improved line intensities for the ν7 band of ethylene near 10.5 μm, and impact on ethylene retrievals from Jungfraujoch solar spectra
Vander Auwera, J; Fayt, A; Tudorie, M et al

in Journal of Quantitative Spectroscopy & Radiative Transfer (2014), 148

Relying on high-resolution Fourier transform infrared (FTIR) spectra, the present work involved extensive measurements of individual line intensities and self broadening coefficients for the nu7 band of ... [more ▼]

Relying on high-resolution Fourier transform infrared (FTIR) spectra, the present work involved extensive measurements of individual line intensities and self broadening coefficients for the nu7 band of 12C2H4. The measured self broadening coefficients exhibit a dependence on both J and Ka. Compared to the corresponding information available in the latest edition of the HITRAN spectroscopic database, the measured line intensities were found to be higher by about 10 % for high J lines in the P branch and lower by about 5 % for high J lines of the R branch, varying between these two limits roughly linearly with the line positions. The impact of the presently measured line intensities on retrievals of atmospheric ethylene in the 949.0-952.0 cm-1 microwindow was evaluated using a subset of ground-based high-resolution FTIR solar spectra recorded at the Jungfraujoch station. The use of HITRAN 2012 with line intensities modified to match the present measurements led to a systematic reduction of the measured total columns of ethylene by -4.1+/-0.1 %. [less ▲]

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See detailSelf broadening coefficients and improved line intensities for the n7 band of C2H4 near 10.5 mm, and impact on ethylene retrievals from Jungfraujoch solar spectra
Vander Auwera, Jean; Fayt, André; Tudorie, Marcela et al

Poster (2014, July 10)

Ethylene (ethene, C2H4) is a tropospheric pollutant on the Earth, also present as a by-product of methane photochemistry in the atmosphere of outer solar system bodies. Remote sensing of ethylene in the ... [more ▼]

Ethylene (ethene, C2H4) is a tropospheric pollutant on the Earth, also present as a by-product of methane photochemistry in the atmosphere of outer solar system bodies. Remote sensing of ethylene in the infrared range relies on the 10 mm region. This spectral range corresponds to the excitation of 7 modes of vibration of 12C2H4, 4 of which being infrared active (see Fig. 1 of [1]). The corresponding n10, n7, n4 and n12 bands are located near 826, 949, 1026 and 1442 cm-1, respectively [1]. Among these, the n7 band is the strongest, indeed used for remote sensing measurements of ethylene. Relying on high-resolution Fourier transform infrared (FTIR) spectra recorded in Brussels, the present work involved extensive measurements of individual line intensities and self broadening coefficients for the n7 band of 12C2H4. Compared to the corresponding information available in the latest edition of the HITRAN spectroscopic database (HITRAN 2012 [2]), the measured line intensities were found to be higher by about 10 % for high J lines in the P branch and lower by about 5 % for high J lines of the R branch, varying between these two limits roughly linearly with the line positions. Test calculations performed in this work indicated that these discrepancies could result from the relative values of the transition moments of the n10, n7 and n12 bands used when the information provided in HITRAN was generated (the transition moment of the n4 band was set to zero). The measured self broadening coefficients exhibit a dependence on both J and Ka, which was modeled empirically. The spectroscopic information for ethylene available in HITRAN 2012 was modified to match the present observations. The impact of these modifications on retrievals of atmospheric ethylene was then evaluated via FTIR retrievals in the 949.0 – 952.0 cm-1 microwindow, from a subset of ground-based high-resolution FTIR solar spectra recorded at the Jungfraujoch station. The new line intensities were found to lead to a reduction of the measured total columns of ethylene by -4.1±0.1 %, compared to the use of HITRAN 2012. [less ▲]

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See detailCarbon monoxide retrieved from ground based FTIR remote sensing in the mid-­‐ and near infrared spectral region
Petri, Christof; Blumenstock, Thomas; Hase, Frank et al

Conference (2014, May 14)

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See detailLong-term evolution and seasonal modulation of methanol 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 ▲]

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See detailSeeking for causes of recent methane increase: comparison between GEOS-Chem tagged simulations and FTIR column measurements above Jungfraujoch
Bader, Whitney ULg; Bovy, Benoît ULg; Wecht, K et al

Poster (2014, May)

Atmospheric CH4 reached 260% of the pre-industrial level (~700 ppb) due to increased emissions from anthropogenic sources. Globally averaged CH4 reached a new high of 1819 ± 1 ppb in 2012, an increase of ... [more ▼]

Atmospheric CH4 reached 260% of the pre-industrial level (~700 ppb) due to increased emissions from anthropogenic sources. Globally averaged CH4 reached a new high of 1819 ± 1 ppb in 2012, an increase of 6 ppb with respect to the previous year (WMO, Greenhouse gas Bulletin N.9, 2013). CH4 above Jungfraujoch increases at 0.53±0.19%/year during the late 90s to stabilize and reach a non significant trend from 2000 to 2005. Since 2006, atmospheric methane has been continuously increasing with a rate of 0.19±0.05 %/year. The attribution of this increase to any CH4 source is difficult since the current network is insufficient to characterize emissions by region and source process, emphasizing the need for source-tagged model simulations as it should provide us information on processes causing the increase of atmospheric methane since 2005/2006. [less ▲]

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See detailRetrieval of HCHO from MAX-DOAS measurements at the high-altitude alpine station of Jungfraujoch (46.5°N, 8.0°E)
Hendrick, François; Fayt, Caroline; Franco, Bruno ULg et al

Conference (2014, April 30)

Formaldehyde (HCHO) plays an important intermediate role in the atmospheric photo-oxidation pathways. It is produced during the oxidation of methane and many non-methane volatile organic compounds (NMVOCs ... [more ▼]

Formaldehyde (HCHO) plays an important intermediate role in the atmospheric photo-oxidation pathways. It is produced during the oxidation of methane and many non-methane volatile organic compounds (NMVOCs) which participate to the formation of tropospheric ozone and secondary organic aerosols. HCHO is also directly released by biomass burning and fossil fuel combustion and to a lesser extent by vegetation. Measuring this species is therefore of major importance for air quality and climate change monitoring. In this presentation, HCHO near-surface concentrations and vertical column densities are retrieved from MAX-DOAS measurements performed at the high-altitude station of Jungfraujoch (3580m asl) in the Swiss Alps from July 2010 till December 2012. Although being most of the time located in the free troposphere, this station can be temporarily affected by pollution events originating from the valley, leading to a local increase of air pollutant concentrations. The capability of the MAX-DOAS technique to retrieve HCHO in such high-altitude location is investigated. The spatial representativeness and the impact of cloud cover on the measurements is also discussed. For verification purpose, our retrievals are compared to collocated FTIR observations, taking into account the difference in vertical resolution between both techniques. Simulations from the 3D-CTM IMAGES are also used to further assess the observed seasonal and diurnal cycles of HCHO surface concentration and vertical column. [less ▲]

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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 ▲]

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See detailRecent results from long-term FTIR monitoring activities at Jungfraujoch: some unexpected trends and new target species
Mahieu, Emmanuel ULg

Scientific conference (2014, January)

Recent results derived from the long-term FTIR monitoring activities conducted by the University of Liège at the Jungfraujoch station are presented, with a focus on new target species.

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See detailRecent increases in Stratospheric HCl: Stratospheric Dynamics versus the Montreal Protocol
Chipperfield, M.P.; Mahieu, Emmanuel ULg; Notholt, J. et al

in Geophysical Research Abstracts (2014), 16

Long-lived chlorine-containing source gases, such as chlorofluorocarbons (CFCs), are transported into the stratosphere where they decompose and cause ozone depletion. Increases in chlorine during the ... [more ▼]

Long-lived chlorine-containing source gases, such as chlorofluorocarbons (CFCs), are transported into the stratosphere where they decompose and cause ozone depletion. Increases in chlorine during the 1970s-1990s resulted in long-term ozone decreases, especially in the polar regions. Following the implementation of the Montreal Protocol, the near-surface chlorine loading was observed to peak in 1993 and, since then, to decrease in line with expectations. After release from source gases in the stratosphere, chlorine mainly forms the reservoir HCl, providing an alternative method for monitoring the progress of the Montreal Protocol. A maximum in stratospheric HCl was observed around 1996, followed by decay at a rate close to 1%/year, consistent with the tropospheric chlorine peak and known transport timescales. However, we will present total column observations from ground-based FTIR instruments which show an unexpected and significant upturn in stratospheric HCl around 2007 in the northern hemisphere. Height-resolved observations from satellite instruments (HALOE, MLS, ACE) confirm this increase and show that it occurs in the lower stratosphere. These observations contrast with the ongoing monotonic decrease of near-surface chlorine source gases. Using 3-D model simulations (TOMCAT/SLIMCAT and KASIMA) we attribute this trend anomaly to a slowdown in the NH atmospheric circulation, causing air in the lower stratosphere to become more aged with a larger relative conversion of source gases to HCl. An important conclusion is that the Montreal Protocol is still on track and will still lead to long-term decreases in stratospheric chlorine. This dynamical variability could also significantly affect the evolution of stratospheric ozone and must be accounted for when searching for signs of ozone recovery. [less ▲]

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See detailPas d'image fiable de notre atmosphère sans mesures depuis le sol !
De Mazière, M; De Backer, H; Mahieu, Emmanuel ULg et al

Article for general public (2014)

Nous sommes actuellement confrontés à une atmosphère en évolution : les concentrations de ce qu’on appelle les gaz à effet de serre augmentent, la quantité d’ozone stratosphérique diminue, en particulier ... [more ▼]

Nous sommes actuellement confrontés à une atmosphère en évolution : les concentrations de ce qu’on appelle les gaz à effet de serre augmentent, la quantité d’ozone stratosphérique diminue, en particulier au-dessus de l’Antarctique où elle forme chaque année un ‘trou’ dans la couche d’ozone, et l’air n’est pas tous les jours très sain... Comment pouvons-nous détecter et surveiller ces changements pour, si nécessaire, prendre des mesures pour tenter de les contrecarrer ? [less ▲]

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See detailComparison of continuous background in-situ and column integrated CO2 observations at Jungfraujoch with an urban site in the city of Bern
Schibig, Michael; Leuenberger, Markus; Nyfeler, Peter et al

in Geophysical Research Abstracts (2014), 16

A six and a half year (January 2005 to May 2011) comparison of CO2 concentration observations has been performed at Jungfraujoch, Switzerland and the city of Bern using two different measurement ... [more ▼]

A six and a half year (January 2005 to May 2011) comparison of CO2 concentration observations has been performed at Jungfraujoch, Switzerland and the city of Bern using two different measurement techniques run by the University of Bern (UBE) and the University of Liege (UL). The UBE systems at Jungfraujoch and Bern are both combined systems for atmospheric oxygen and CO2 measurements. The cryogenically dried air is analysed for CO2 with a Maihak analyser based on the broad-band infrared absorption technique. The measurement frequency is every second but the final reported data are averages of six minute periods. UL is measuring the solar infrared spectrum since 1950 at Jungfraujoch. On its way through the atmosphere, the solar spectrum is modulated depending on the abundant gas species and their amount in the column. Since some gases like CO2 absorb the solar infrared radiation at particular wavelengths and the extinction is proportional to the gas concentration, it is possible to determine the gas concentration in the column above the sensor. At the conference, we will present the three observational records for the six and a half year period. The results show for all three records a distinct, but different seasonality. The seasonalities of the UL and UBE record at Jungfraujoch are lower than the seasonality in the city of Bern, i.e. 4.5 ppm per year and 9 ppm per year for the column and the in- situ record respectively, whereas the seasonality in the city of Bern is 31 ppm per year. Also the maxima and minima of the Jungfraujoch measurements are delayed by several weeks compared to the measurements in the city of Bern. The annual increase of the CO2 concentration of the UBE and UL records of Jungfraujoch are in good agreement with 1.94 ppm per year and 1.90 ppm per year, respectively. The annual increase of the CO2 concentration at the urban site is a bit higher at 2.01 ppm per year. [less ▲]

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See detailValidation of ACE-FTS measurements of CFC-11, CFC-12 and HCFC-22 using ground-based FTIRs
Kolonjari, F; Walker, K A; Mahieu, Emmanuel ULg et al

Poster (2013, December 10)

Satellite data can be an effective global monitoring tool for long-lived compounds in the atmosphere. The Atmospheric Chemistry Experiment (ACE) is a mission onboard 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 onboard 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 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 (CCl3F), CFC-12 (CCl2F2), and HCFC-22 (CHClF2) retrieved profiles from ACE-FTS measurements. These species are related because HCFC-22 was the primary replacement for CFC-11 and CFC-12 in refrigerant and propellant applications. The FTIRs used in this study record solar absorption spectra at Eureka (Canada), Jungfraujoch (Switzerland), Poker Flat (USA), and Toronto (Canada). The retrieval of CFC-11, CFC-12, and HCFC-22 are not standard products for many of these FTIRs, and as such, a harmonization of retrieval parameters between the sites has been conducted. The retrievals of these species from the FTIR spectra are sensitive from the surface to approximately 20 km, while the ACE-FTS profiles extend from 6 to 30 km. For each site, partial column comparisons between coincident measurements of the three species and a validation of the observed trends will be discussed. [less ▲]

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See detailParallel measurements of formaldehyde (H2CO) at the Jungfraujoch station: preliminary FTIR results and first comparison with Max-DOAS data
Franco, Bruno ULg; Mahieu, Emmanuel ULg; Van Roozendael, Michel et al

Conference (2013, October 17)

In the framework of the NORS project, a retrieval strategy for formaldehyde (H2CO) is currently under development, using measurements from ground-based high-resolution FTIR solar spectra recorded at the ... [more ▼]

In the framework of the NORS project, a retrieval strategy for formaldehyde (H2CO) is currently under development, using measurements from ground-based high-resolution FTIR solar spectra recorded at the NDACC high altitude station of the Jungfraujoch (Swiss Alps, 46.5° N, 8.0° E, 3580m a.s.l.). According to the preliminary results, our FTIR retrieval strategy based on Tikhonov regularization has proven able to make an improvement in the process of fitting the H2CO feature within the 2833.070 – 2833.350 cm-1 microwindow from Jungfraujoch solar spectra, compared to a simple scaling. Furthermore, the retrieved total columns present a seasonal cycle averaged over 2005 – 2013 in agreement with preliminary results from UV-visible MAX-DOAS observations, ACE-FTS occultation measurements and simulations from the IMAGES and GEOS-CHEM models. However, FTIR H2CO abundances appear to be underestimated during summertime, with respect to the other data sets. In order to solve this issue, further experiments are planned. [less ▲]

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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 detailMeasurements of hydrogen cyanide (HCN) and acetylene (C2H2) from the Infrared Atmospheric Sounding Interferometer (IASI)
Duflot, V.; Hurtmans, D.; Clarisse, L. et al

in Atmospheric Measurement Techniques (2013), 6

Hydrogen cyanide (HCN) and acetylene (C2H2) are ubiquitous atmospheric trace gases with medium lifetime, which are frequently used as indicators of combustion sources and as tracers for atmospheric ... [more ▼]

Hydrogen cyanide (HCN) and acetylene (C2H2) are ubiquitous atmospheric trace gases with medium lifetime, which are frequently used as indicators of combustion sources and as tracers for atmospheric transport and chemistry. Because of their weak infrared absorption, overlapped by the CO2 Q branch near 720 cm−1, nadir sounders have up to now failed to measure these gases routinely. Taking into account CO2 line mixing, we provide for the first time extensive measurements of HCN and C2H2 total columns at Reunion Island (21° S, 55° E) and Jungfraujoch (46° N, 8° E) in 2009–2010 using observations from the Infrared Atmospheric Sounding Interferometer (IASI). A first order comparison with local ground-based Fourier transform InfraRed (FTIR) measurements has been carried out allowing tests of seasonal consistency which is reasonably captured, except for HCN at Jungfraujoch. The IASI data shows a greater tendency to high C2H2 values. We also examine a nonspecific biomass burning plume over austral Africa and show that the emission ratios with respect to CO agree with previously reported values. [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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