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See detailGaz à effet de serre indirects et qualité de l'air aux latitudes moyennes de l'hémisphère nord : tendances à long terme et variabilité déduites de télémesures effectuées au Jungfraujoch (Alpes suisses, 3580 m)
Franco, Bruno ULg; Bader, Whitney ULg; Lejeune, Bernard ULg et al

Conference (2015, July 01)

Indirect greenhouse gases and air quality at Northern Hemisphere mid-latitudes: long-term trends and variability derived from ground-based remote sensing at Jungfraujoch (Swiss Alps, 3580 m a.s.l.). We ... [more ▼]

Indirect greenhouse gases and air quality at Northern Hemisphere mid-latitudes: long-term trends and variability derived from ground-based remote sensing at Jungfraujoch (Swiss Alps, 3580 m a.s.l.). We present an overview of recent investigations conducted by the Solar and Atmospheric Physics Infrared Group at the University of Liège and dedicated to the long-term monitoring of atmospheric gases with an indirect greenhouse effect and affecting air quality at Northern Hemisphere mid-latitudes. Gas concentrations are derived from high-resolution solar spectra recorded at the Jungfraujoch station (Swiss Alps, 46.5° N, 8.0° E, 3580 m a.s.l.), using Fourier transform infrared spectrometers. Time series obtained from these observations, along with satellite measurements and simulations from numerical models, allow for the study of both variability and recent evolution of these species and are critical for air quality monitoring and understanding climate changes. [less ▲]

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See detailRecent ethane increase above North America: comparison between FTIR measurements and model simulations
Franco, Bruno ULg; Bader, Whitney ULg; Mahieu, Emmanuel ULg et al

Conference (2015, June 11)

Ethane (C2H6) has a large impact on tropospheric composition and air quality because of its involvement in the global VOC (volatile organic compound) – HOx – NOx chemistry responsible for generating and ... [more ▼]

Ethane (C2H6) has a large impact on tropospheric composition and air quality because of its involvement in the global VOC (volatile organic compound) – HOx – NOx chemistry responsible for generating and destroying tropospheric ozone. By acting as a major sink for tropospheric OH radicals, the abundance of C2H6 influences the atmospheric content of carbon monoxide and impacts the lifetime of methane. Moreover, it is an important source of PAN, a thermally unstable reservoir for NOx radicals. On a global scale, the main sources of C2H6 are leakage from the production, transport of natural gas loss, biofuel consumption and biomass burning, mainly located in the Northern Hemisphere. Due to its relatively long lifetime of approximately two months, C2H6 is a sensitive indicator of tropospheric pollution and transport. Using an optimized retrieval strategy (see Franco et al., 2014), we present here a 20-year long-term time series of C2H6 column abundance retrieved from ground-based Fourier Transform InfraRed (FTIR) solar spectra recorded from 1994 onwards at the high-altitude station of Jungfraujoch (Swiss Alps, 46.5° N, 3580 m a.s.l.), part of the Network for the Detection of Atmospheric Composition Change (NDACC, see http://www.ndacc.org). After a regular 1994 – 2008 decrease of the C2H6 amounts, which is very consistent with prior major studies (e.g., Aydin et al., 2011; Simpson et al., 2012) and our understanding of global C2H6 emissions, trend analysis using a bootstrap resampling tool reveals a C2H6 upturn and a statistically-significant sharp burden increase from 2009 onwards (Franco et al., 2014). We hypothesize that this observed recent increase in C2H6 could affect the whole Northern Hemisphere and may be related to the recent massive growth in the exploitation of shale gas and tight oil reservoirs. This hypothesis is supported by measurements derived from solar occultation observations performed since 2004 by the Atmospheric Chemistry Experiment – Fourier Transform Spectrometer (ACE-FTS) instrument and at other NDACC sites, namely Toronto (44° N) and Thule (77° N). Indeed, the recent rates of changes characterizing these data sets are consistent in magnitude and sign with the one derived from the FTIR measurements at Jungfraujoch. In contrast, the ethane time series form Lauder (45° S) shows a monotonic decrease over the last two decades. Investigating both the cause and impact on air quality of the C2H6 upturn should be a high priority for the atmospheric chemistry community. [less ▲]

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See detailInvestigation of the consistency of the recent CH4 increase derived from NDACC-FTIR, ACE-FTS and GEOS-Chem
Bader, Whitney ULg; Conway, Stephanie; Strong, Kim et al

Conference (2015, May 21)

We present an update on the status of the recent methane increase study based on six FTIR ground-based sites, ACE-FTS satellite occultations and GEOS-Chem simulation.

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See detailRecent results derived from regular ground-based FTIR observations at the Jungfraujoch and other NDACC stations
Mahieu, Emmanuel ULg; Bader, Whitney ULg; Franco, Bruno ULg

Scientific conference (2015, May 20)

We present an overview of the recent results derived from the observational program for the long-term monitoring of the Earth's atmosphere from the Jungfraujoch station, including comparison with data ... [more ▼]

We present an overview of the recent results derived from the observational program for the long-term monitoring of the Earth's atmosphere from the Jungfraujoch station, including comparison with data from the ACE-FTS satellite instrument and other NDACC stations. [less ▲]

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See detailUse of GEOS-Chem for the interpretation of long-term FTIR measurements at the Jungfraujoch and other NDACC sites
Mahieu, Emmanuel ULg; Bovy, Benoît ULg; Bader, Whitney ULg et al

Poster (2015, May 04)

We present recent and ongoing investigations using 3D CTM GEOS-Chem model simulations for the interpretation of long-term FTIR measurements performed at selected NDACC sites.

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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 (2015), 8

As an 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 an 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, 3580m a.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), GEOSChem and IMAGES v2, 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 CTM outputs as the 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. Finally, tests have revealed that the updated IR parameters from the HITRAN 2012 database have a cumulative effect and significantly decrease the retrieved HCHO columns with respect to the use of the HITRAN 2008 compilation. [less ▲]

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See detailHalogenated source gases measured by FTIR at the Jungfraujoch station: updated trends and new target species
Mahieu, Emmanuel ULg; Bader, Whitney ULg; Bovy, Benoît ULg et al

in Geophysical Research Abstracts (2015, April 13), 17

In this contribution, we present decadal time series of halogenated source gases monitored at the high altitude station of the Jungfraujoch (46.5°N, 8°E, 3580 m asl) with Fourier Transform Infared (FTIR ... [more ▼]

In this contribution, we present decadal time series of halogenated source gases monitored at the high altitude station of the Jungfraujoch (46.5°N, 8°E, 3580 m asl) with Fourier Transform Infared (FTIR) spectrometers, within the framework of the Network for the Detection of Atmospheric Composition Change. Total column trends presented in previous studies for CFC-11, -12 and HCFC-22, CCl4, HCFC-142b, CF4 and SF6 will be updated using the latest available Jungfraujoch solar observations. Investigations dealing with the definition of approaches to retrieve additional halogenated source gases from FTIR spectra will also be evoked. Our trend results will be critically discussed and compared with measurements performed in the northern hemisphere by the in situ networks. [less ▲]

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See detailRecent increase of ethane detected in the remote atmosphere of the Northern Hemisphere
Franco, Bruno ULg; Bader, Whitney ULg; Bovy, Benoît ULg et al

Conference (2015, April 13)

Ethane (C2H6) has a large impact on tropospheric composition and air quality because of its involvement in the global VOC (volatile organic compound) – HOx – NOx chemistry responsible for generating and ... [more ▼]

Ethane (C2H6) has a large impact on tropospheric composition and air quality because of its involvement in the global VOC (volatile organic compound) – HOx – NOx chemistry responsible for generating and destroying tropospheric ozone. By acting as a major sink for tropospheric OH radicals, the abundance of C2H6 influences the atmospheric content of carbon monoxide and impacts the lifetime of methane. Moreover, it is an important source of PAN, a thermally unstable reservoir for NOx radicals. On a global scale, the main sources of C2H6 are leakage from the production, transport of natural gas loss, biofuel consumption and biomass burning, mainly located in the Northern Hemisphere. Due to its relatively long lifetime of approximately two months, C2H6 is a sensitive indicator of tropospheric pollution and transport. Using an optimized retrieval strategy (see Franco et al., 2014), we present here a 20-year long-term time series of C2H6 column abundance retrieved from ground-based Fourier Transform InfraRed (FTIR) solar spectra recorded from 1994 onwards at the high-altitude station of Jungfraujoch (Swiss Alps, 46.5° N, 3580 m a.s.l.), part of the Network for the Detection of Atmospheric Composition Change (NDACC, see http://www.ndacc.org). After a regular 1994 – 2008 decrease of the C2H6 amounts, which is very consistent with prior major studies (e.g., Aydin et al., 2011; Simpson et al., 2012) and our understanding of global C2H6 emissions, trend analysis using a bootstrap resampling tool reveals a C2H6 upturn and a statistically-significant sharp burden increase from 2009 onwards (Franco et al., 2014). We hypothesize that this observed recent increase in C2H6 could affect the whole Northern Hemisphere and may be related to the recent massive growth in the exploitation of shale gas and tight oil reservoirs. This hypothesis is supported by measurements derived from solar occultation observations performed since 2004 by the Atmospheric Chemistry Experiment – Fourier Transform Spectrometer (ACE-FTS) instrument and at other NDACC sites, namely Toronto (44° N) and Thule (77° N). Indeed, the recent rates of changes characterizing these data sets are consistent in magnitude and sign with the one derived from the FTIR measurements at Jungfraujoch. In contrast, the ethane time series form Lauder (45° S) shows a monotonic decrease over the last two decades. Investigating both the cause and impact on air quality of the C2H6 upturn should be a high priority for the atmospheric chemistry community. [less ▲]

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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 (2015), 160(C), 36-49

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 detailUne nouvelle menace pour la couche d'ozone ?
Franco, Bruno ULg

Scientific conference (2014, December 04)

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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 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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