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See detailRetrievals of ethane from ground-based high-resolution FTIR solar observations with updated line parameters: determination of the optimum strategy for the Jungfraujoch station.
Bader, Whitney ULg; Perrin, Agnès; Jacquemart, David et al

Poster (2012, August)

Ethane (C2H6) is the most abundant Non-Methane HydroCarbon (NMHC) in the Earth’s atmosphere, with a lifetime of approximately 2 months. C2H6 has both anthropogenic and natural emission sources such as ... [more ▼]

Ethane (C2H6) is the most abundant Non-Methane HydroCarbon (NMHC) in the Earth’s atmosphere, with a lifetime of approximately 2 months. C2H6 has both anthropogenic and natural emission sources such as biomass burning, natural gas loss and biofuel consumption. The retrieval of ethane from ground-based infrared spectra is challenging. Indeed, ethane has a complicated spectrum with many interacting vibrational modes and the current state of ethane parameters in HITRAN (see http://www.hitran.com) was rather unsatisfactory in the 3 μm region. In fact, PQ branches outside the 2973–3001 cm-1 range are not included in HITRAN, and most P and R structures are missing. New ethane absorption cross sections recorded at the Molecular Spectroscopy Facility of the Rutherford Appleton Laboratory (Harrison et al., 2010) are used in our retrievals. Pseudoline parameters fitted to these ethane spectra have been combined with HITRAN 2004 line parameters (including all the 2006 updates) for all other species encompassed in the selected microwindows. We evaluated the impact on spectral residuals induced by the update of two O3 lines (encompassed in the PQ3 µ-window) corrected by P. Chelin (LPMA, Paris, France). We also quantified the improvement brought by the update of the line positions and intensities of methyl chloride (CH3Cl) in the 3.4 µm region (Bray et al., 2011). The ethane a priori volume mixing ratio (VMR) profile and associated covariance are based on synthetic data from CHASER 3-D chemical transport model (CTM). In this contribution, we will present updated ethane (total) column retrievals, using the SFIT-2 algorithm (v3.91) and high-resolution Fourier Transform Infrared (FTIR) solar absorption observations recorded with a Bruker 120HR instrument, at the high altitude research station of the Jungfraujoch (46.5°N, 8°E, 3580 m asl), within the framework of the Network for the Detection of Atmospheric Composition Change (NDACC, visit http://www.ndacc.org). Comparisons with synthetic data produced by two chemical transport models (CHASER and the one of the University of Oslo) will also be presented and analyzed, aiming at the determination and interpretation of long-term trends and interannual variations of ethane at Northern mid-latitudes. [less ▲]

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See detailRetrievals of ethane from groundbased highresolution FTIR solar observations with updated line parameters: determination of the optimum strategy for the Jungfraujoch station.
Bader, Whitney ULg; Perrin, Agnès; Jacquemart, David et al

Scientific conference (2012, June 01)

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

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

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See 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

in Geophysical Research Abstracts (2012), 14(EGU2012-9126),

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. Oxidation by the hydroxyl radical is by far the major C2H6 sink as the seasonally changing OH concentration controls the strong modulation of the ethane abundance throughout the year. Ethane lowers Cl atom concentrations in the lower stratosphere and is a major source of peroxyacetyl nitrate (PAN) and carbon monoxide (by reaction with OH). Involved in the formation of tropospheric ozone and in the destruction of atmospheric methane through changes in OH, C2H6 is a non-direct greenhouse gas with a net-global warming potential (100-yr horizon) of 5.5. The retrieval of ethane from ground-based infrared (IR) spectra is challenging. Indeed, the fitting of the ethane features is complicated by numerous interferences by strong water vapor, ozone and methane absorptions. Moreover, ethane has a complicated spectrum with many interacting vibrational modes and the current state of ethane parameters in HITRAN (e.g. : Rothman et al., 2009, 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. They were calibrated in intensity by using reference low-resolution spectra from the Pacific Northwest National Laboratory (PNNL) IR database. 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. Also, the improvement brought by the update of the line positions and intensities of methyl chloride (CH3Cl) in the 3.4 m region (Bray et al., 2011) will be quantified. The ethane a priori volume mixing ratio (VMR) profile and associated covariance are based on synthetic data from the chemical transport model (CTM) of the University of Oslo. In this contribution, we will present updated ethane total and tropospheric 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). We will characterize three microwindows encompassing the strongest ethane features after careful selection of a priori VMR profiles, spectroscopic parameters, accounting at best for all interfering species. We will then present the retrieval strategy representative of the best combination of those three characterized micro-windows in order to minimize the fitting residuals while maximizing the information content, the precision and the reliability of the retrieved product. The long-term C2H6 column time series will be produced using the Jungfraujoch observational database. Comparisons with synthetic data produced by two chemical transport model (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 detailExtension of the long-term total column time series of atmospheric methane above the Jungfraujoch station: analysis of grating infrared spectra between 1976 and 1989
Bader, Whitney ULg; Lejeune, Bernard ULg; Demoulin, Philippe ULg et al

in Geophysical Research Abstracts (2011), 13

Methane (CH4) is one of the most abundant greenhouse gases in the Earth’s atmosphere, with current mean volume mixing ratio close to 1800 ppb. Since methane has a global warming potential of 25 (100-yr ... [more ▼]

Methane (CH4) is one of the most abundant greenhouse gases in the Earth’s atmosphere, with current mean volume mixing ratio close to 1800 ppb. Since methane has a global warming potential of 25 (100-yr horizon) and an atmospheric lifetime of 12 years, the Kyoto Protocol has included it among the species to be regulated to limit global warming. Anthropogenic sources of methane are mainly energy production (coal and leaks) and agriculture while main natural sources are swamps and biomass waste. The main sink of methane is oxidation in the troposphere, primarily by reaction with the hydroxyl radical. Methane trends have exhibited significant changes during the last twenty-five years. For instance, long-term monitoring of its vertical total column above the high-altitude station of the Jungfraujoch (46.5°N, 8°E, 3580 m asl) has indeed allowed to derive column changes ranging from +0.72% in 1987-1988 to +0.14% in 1999-2000 (Zander et al., 2002), relative to 1988 and 2000, respectively. More recently and for the same site, Duchatelet et al. (2010) have even reported a significant slowdown of -0.02%/yr between years 2000 and 2005. This study also showed that since then, CH4 is on the rise again, at a rate close to +0.30%/yr. While the numbers reported here above have been derived from the Fourier Transform Infrared (FTIR) data set starting in 1984, earlier pioneering observations have been collected at the Jungfraujoch since 1950, using grating spectrometers. During the 1958-1975 period, the main objectives has been the study of the solar photosphere in the visible and the near infrared and the publication of high-resolution solar atlases. From 1976 to 1989, narrow-band IR solar absorption observations achieving a spectral resolution of about 0.02 cm-1 have been recorded with the high-performance double-pass grating spectrometer. Analysis of these historical spectra provides a unique opportunity to extend the Jungfraujoch’s total column time series of important atmospheric gases, including methane, by nearly 10 years. The aim of this contribution is to present the inversion strategy adopted to derive CH4 from the grating spectra, using the SFIT-2 algorithm (v3.91) We will evaluate the impact of resolution, spectroscopic parameters (from the EU HYMN project -see www.knmi.nl/samen/hymn-, and from HITRAN 2004), atmospheric pressure and temperature profiles on the error budget. The 1976-1989 total column time series produced will be presented and critically discussed. In particular, we will identify and correct for possible biases between double-pass grating spectrometer measurements and more recent FTIR total columns. The harmonized and consolidated time series will be investigated to characterize the long-term trend of methane for the 1976-2010 time period. Comparisons with synthetic data produced by the CHASER 3-dimensional chemical transport model will also be presented and analyzed. [less ▲]

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