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See detailRetrieval of ethane from ground-based FTIR solar spectra using improved spectroscopy: recent burden increase above Jungfraujoch
Franco, Bruno ULg; Bader, Whitney ULg; Toon, G. C. et al

in Journal of Quantitative Spectroscopy & Radiative Transfer (in press)

An improved spectroscopy is used to implement and optimize the retrieval strategy of ethane (C2H6) from ground-based Fourier Transform Infrared (FTIR) solar spectra recorded at the high-altitude station ... [more ▼]

An improved spectroscopy is used to implement and optimize the retrieval strategy of ethane (C2H6) from ground-based Fourier Transform Infrared (FTIR) solar spectra recorded at the high-altitude station of Jungfraujoch (Swiss Alps, 46.5° N, 8.0° E, 3580m a.s.l.). The improved spectroscopic parameters include C2H6 pseudo-lines in the 2720-3100 cm-1 range and updated line parameters for methyl chloride and ozone. These improved spectroscopic parameters allow for substantial reduction of the fitting residuals as well as enhanced information content. They also contribute to limiting oscillations responsible for ungeophysical negative mixing ratio profiles. This strategy has been successfully applied to the Jungfraujoch solar spectra available from 1994 onwards. The resulting time series is compared with C2H6 total columns simulated by the state-of-the-art chemical transport model GEOS-Chem. Despite very consistent seasonal cycles between both data sets, a negative systematic bias relative to the FTIR observations suggests that C2H6 emissions are underestimated in the current inventories implemented in GEOS-Chem. Finally, C2H6 trends are derived from the FTIR time series, revealing a statistically-significant sharp increase of the C2H6 burden in the remote atmosphere above Jungfraujoch since 2009. Evaluating cause of this change in the C2H6 burden, which may be related to the recent massive growth of shale gas exploitation in North America, is of primary importance for atmospheric composition and air quality in the Northern Hemisphere. [less ▲]

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See detailUsing XCO2 retrievals for assessing the long-term consistency of NDACC/FTIR data sets
Barthlott, S; Schneider, M; Hase, F et al

in Atmospheric Measurement Techniques (2015), 8

Within the NDACC (Network for the Detection of Atmospheric Composition Change), more than 20 FTIR (Fourier-transform infrared) spectrometers, spread worldwide, provide long-term data records of many ... [more ▼]

Within the NDACC (Network for the Detection of Atmospheric Composition Change), more than 20 FTIR (Fourier-transform infrared) spectrometers, spread worldwide, provide long-term data records of many atmospheric trace gases. We present a method that uses measured and modelled XCO2 for assessing the consistency of these NDACC data records. Our XCO2 retrieval setup is kept simple so that it can easily be adopted for any NDACC/FTIR-like measurement made since the late 1950s. By a comparison to coincident TCCON (Total Carbon Column Observing Network) measurements, we empirically demonstrate the useful quality of this suggested NDACC XCO2 product (empirically obtained scatter between TCCON and NDACC is about 4‰ for daily mean as well as monthly mean comparisons, and the bias is 25 ‰). Our XCO2 model is a simple regression model fitted to CarbonTracker results and the Mauna Loa CO2 in situ records. A comparison to TCCON data suggests an uncertainty of the model for monthly mean data of below 3 ‰. We apply the method to the NDACC/FTIR spectra that are used within the project MUSICA (multi-platform remote sensing of isotopologues for investigating the cycle of atmospheric water) and demonstrate that there is a good consistency for these globally representative set of spectra measured since 1996: the scatter between the modelled and measured XCO2 on a yearly time scale is only 3 ‰. [less ▲]

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See detailPast changes in the vertical distribution of ozone – Part 3: Analysis and interpretation of trends
Harris, N. R. P.; Hassler, B.; Tummon, F. et al

in Atmospheric Chemistry & Physics Discussions (2015), 15(6), 8565--8608

Trends in the vertical distribution of ozone are reported and compared for a number of new and recently revised datasets. The amount of ozone-depleting compounds in the stratosphere (as measured by ... [more ▼]

Trends in the vertical distribution of ozone are reported and compared for a number of new and recently revised datasets. The amount of ozone-depleting compounds in the stratosphere (as measured by Equivalent Effective Stratospheric Chlorine – EESC) maximised in the second half of the 1990s. We therefore examine the trends in the periods before and after that peak to see if any change in trend is discernible in the ozone record. Prior to 1998, trends in the upper stratosphere (~ 45 km, 4 hPa) are found to be −5 to −10% per decade at mid-latitudes and closer to −5% per decade in the tropics. No trends are found in the mid-stratosphere (28 km, 30 hPa). Negative trends are seen in the lower stratosphere at mid-latitudes in both hemispheres and in the deep tropics. However it is hard to be categorical about the trends in the lower stratosphere for three reasons: (i) there are fewer measurements, (ii) the data quality is poorer, and (iii) the measurements in the 1990s are perturbed by aerosols from the Mt. Pinatubo eruption in 1991. These findings are similar to those reported previously even though the measurements for the two main satellite instruments (SBUV and SAGE II) and the ground-based Umkehr and ozonesonde stations have been revised. There is no sign of a continued negative trend in the upper stratosphere since 1998: instead there is a hint of an average positive trend of ~ 2% per decade in mid-latitudes and ~ 3% per decade in the tropics. The significance of these upward trends is investigated using different assumptions of the independence of the trend estimates found from different datasets. The averaged upward trends are significant if the trends derived from various datasets are assumed to be independent, but are generally not significant if the trends are not independent. This arises because many of the underlying measurement records are used in more than one merged dataset. At this point it is not possible to say which assumption is best. Including an estimate of the drift of the overall ozone observing system decreases the significance of the trends. The significance will become clearer as (i) more years are added to the observational record, (ii) further improvements are made to the historic ozone record (e.g. through algorithm development), and (iii) the data merging techniques are refined, particularly through a more rigorous treatment of uncertainties. [less ▲]

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See detailTrends of ozone total columns and vertical distribution from FTIR observations at eight NDACC stations around the globe
Vigouroux, C; Blumenstock, T; Coffey, M et al

in Atmospheric Chemistry and Physics (2015), 15

Ground-based Fourier transform infrared (FTIR) measurements of solar absorption spectra can provide ozone total columns with a precision of 2 % but also independent partial column amounts in about four ... [more ▼]

Ground-based Fourier transform infrared (FTIR) measurements of solar absorption spectra can provide ozone total columns with a precision of 2 % but also independent partial column amounts in about four vertical layers, one in the troposphere and three in the stratosphere up to about 45 km, with a precision of 5–6 %. We use eight of the Network for the Detection of Atmospheric Composition Change (NDACC) stations having a long-term time series of FTIR ozone measurements to study the total and vertical ozone trends and variability, namely, Ny-Ålesund (79ºN), Thule (77ºN), Kiruna (68ºN), Harestua (60ºN), Jungfraujoch (47ºN), Izaña (28ºN), Wollongong (34ºS) and Lauder (45ºS). The length of the FTIR time series varies by station but is typically from about 1995 to present. We applied to the monthly means of the ozone total and four partial columns a stepwise multiple regression model including the following proxies: solar cycle, quasi-biennial oscillation (QBO), El Niño–Southern Oscillation (ENSO), Arctic and Antarctic Oscillation (AO/AAO), tropopause pressure (TP), equivalent latitude (EL), Eliassen–Palm flux (EPF), and volume of polar stratospheric clouds (VPSC). At the Arctic stations, the trends are found mostly negative in the troposphere and lower stratosphere, very mixed in the middle stratosphere, positive in the upper stratosphere due to a large increase in the 1995–2003 period, and non-significant when considering the total columns. The trends for mid-latitude and subtropical stations are all non-significant, except at Lauder in the troposphere and upper stratosphere and at Wollongong for the total columns and the lower and middle stratospheric columns where they are found positive. At Jungfraujoch, the upper stratospheric trend is close to significance (+0.9 ± 1.0 %/decade). Therefore, some signs of the onset of ozone mid-latitude recovery are observed only in the Southern Hemisphere, while a few more years seem to be needed to observe it at the northern mid-latitude station. [less ▲]

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See detailUpdate on Ozone-Depleting Substances (ODSs) and Other Gases of Interest to the Montreal Protocol
Carpenter, L. J.; Reimann, S.; Burkholder, J. B. et al

in Nohende Ajavon, Ayité-Lô; Newman, Paul. A.; Pyle, John A. (Eds.) et al Scientific Assessment of Ozone Depletion: 2014 (2014)

The amended and adjusted Montreal Protocol has continued to reduce emissions and atmospheric abundances of most controlled ozone-depleting substances. By 2012, the total combined abundance of ... [more ▼]

The amended and adjusted Montreal Protocol has continued to reduce emissions and atmospheric abundances of most controlled ozone-depleting substances. By 2012, the total combined abundance of anthropogenic ODSs in the troposphere (measured as Equivalent Chlorine) had decreased by nearly 10% from its peak value in 1994. [less ▲]

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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, T; Muller, J-F et al

in Atmospheric Measurement Techniques (2014), 7

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

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

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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 detailValidation of SCIAMACHY HDO/H2O measurements using the TCCON and NDACC-MUSICA networks
Scheepmaker, R. A.; Frankenberg, C.; Deutscher, N. M. et al

in Atmospheric Measurement Techniques. Papers in Open Discussion (2014), 7(11), 11799--11851

Measurements of the atmospheric HDO/H2O ratio help us to better understand the hydrological cycle and improve models to correctly simulate tropospheric humidity and therefore climate change. We present an ... [more ▼]

Measurements of the atmospheric HDO/H2O ratio help us to better understand the hydrological cycle and improve models to correctly simulate tropospheric humidity and therefore climate change. We present an updated version of the column-averaged HDO/H2O ratio dataset from the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY). The dataset is extended with two additional years, now covering 2003–2007, and is validated against co-located ground-based total column delta-D measurements from Fourier-Transform Spectrometers (FTS) of the Total Carbon Column Observing Network (TCCON) and the Network for the Detection of Atmospheric Composition Change (NDACC, produced within the framework of the MUSICA project). Even though the time overlap between the available data is not yet ideal, we determined a mean negative bias in SCIAMACHY delta-D of -35±30‰ compared to TCCON and -69±15‰ compared to MUSICA (the uncertainty indicating the station-to-station standard deviation). The bias shows a latitudinal dependency, being largest (about -60 to -80‰) at the highest latitudes and smallest (about -20 to -30‰) at the lowest latitudes. We have tested the impact of an offset correction to the SCIAMACHY HDO and H2O columns. This correction leads to a humidity and latitude dependent shift in delta-D and an improvement of the bias by 27 ‰, although it does not lead to an improved correlation with the FTS measurements nor to a strong reduction of the latitudinal dependency of the bias. The correction might be an improvement for dry, high-altitude areas, such as the Tibetan Plateau and the Andes region. For these areas, however, validation is currently impossible due to a lack of ground stations. The mean standard deviation of single-sounding SCIAMACHY–FTS differences is ~115 ‰, which is reduced by a factor ~2 when we consider monthly means. When we relax the strict matching of individual measurements and focus on the mean seasonalities using all available FTS data, we find that the correlation coefficients between SCIAMACHY and the FTS networks improve from 0.2 to 0.7–0.8. Certain ground stations show a clear asymmetry in delta-D during the transition from the dry to the wet season and back, which is also detected by SCIAMACHY. This asymmetry points to a transition in the source region temperature or location of the water vapor, and shows the added information that HDO/H2O measurements provide, if used in combination with variations in humidity. [less ▲]

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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

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

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. In this study, HCHO profiles have been successfully retrieved 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, 3580ma.s.l.). Analysis 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 the HCHO retrieval above the Jungfraujoch station. [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 detailImproved spectral fitting of nitrogen dioxide from OMI in the 405-465 nm window
van Geffen, J H G M; Boersma, K F; Van Roozendael, M et al

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

An improved nitrogen dioxide (NO2) slant column density retrieval for the Ozone Monitoring Instrument (OMI) in the 405–465 nm spectral region is presented. Since the launch of OMI on board NASA's EOS-Aura ... [more ▼]

An improved nitrogen dioxide (NO2) slant column density retrieval for the Ozone Monitoring Instrument (OMI) in the 405–465 nm spectral region is presented. Since the launch of OMI on board NASA's EOS-Aura satellite in 2004, DOAS retrievals of NO2 slant column densities have been the starting point for the KNMI DOMINO (v2.0) and NASA SP (v2.1) retrievals. However, recent intercomparisons between NO2 retrievals from OMI and other UV/Vis and limb spectrometers, as well as ground-based measurements, clearly suggested that OMI stratospheric NO2 is biased high. This study revises the OMI NO2 retrieval in detail. The representation of the OMI slit function to convolve high-resolution reference spectra onto the relevant spectral grid is improved. The window used for the wavelength calibration is optimised, leading to much-reduced fitting errors. Ozone and water vapour spectra used in the fit are updated, reflecting the recently improved knowledge on their absorption cross section as documented in the literature. The improved spectral fit also accounts for absorption by the O2–O2 collision complex and by liquid water over clear-water areas. The main changes in the improved spectral fitting result from the updates related to the wavelength calibration: the RMS error of the fit is reduced by 23% and the NO2 slant column by 0.85 × 1015 molec cm-2, independent of latitude, solar zenith angle and NO2 value. Including O2–O2 and liquid water absorption and updating the O3 and water vapour cross-section spectra further reduces NO2 slant columns on average by 0.35 × 1015 molec cm-2, accompanied with a further 9% reduction in the RMS error of the fit. The improved OMI NO2 slant columns are consistent with independent NO2 retrievals to within a range that can be explained by photo-chemically driven diurnal increases in stratospheric NO2 and by small differences in fitting window and fitting approach. The revisions indicate that current OMI NO2 slant columns suffered mostly from an additive, positive offset that is removed by the improved wavelength calibration and representation of the OMI slit function. It is therefore anticipated that the improved NO2 slant columns are most important to retrievals of spatially homogeneous stratospheric NO2 rather than to heterogeneous tropospheric NO2. [less ▲]

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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 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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