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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 detailOzone tropospheric and stratospheric trends (1995-2012) at six ground-based FTIR stations (28°N to 79°N)
Vigouroux, Corinne; De Mazière, Martine; Demoulin, Philippe ULg et al

Poster (2013, April)

In the frame of the Network for the Detection of Atmospheric Composition Change (NDACC), contributing ground-based stations have joined their efforts to homogenize and optimize the retrievals of ozone ... [more ▼]

In the frame of the Network for the Detection of Atmospheric Composition Change (NDACC), contributing ground-based stations have joined their efforts to homogenize and optimize the retrievals of ozone profiles from FTIR (Fourier transform infrared) solar absorption spectra. Using the optimal estimation method, distinct vertical information can be obtained in four layers: ground-10 km, 10-18 km, 18-27 km, and 27-42 km, in addition to total column amounts. In a previous study, Vigouroux et al. (2008) applied a bootstrap resampling method to determine the trends of the ozone total and four partial columns, over the period 1995-2004 at Western European stations. The updated trends for the period 1995-2009 have been published in the WMO 2010 report. Here, we present the updated trends and their uncertainties, for the 1995-2012 period, for the different altitude ranges, above five European stations (28°N-79°N) and above the station Thule, Greenland (77°N). In this work, the trends have been estimated using a multiple regression model including some explanatory variables responsible for the ozone variability, such as the Quasi Biennial Oscillation (QBO), the solar flux, the Arctic Oscillation (AO) or El Niño-Southern Oscillation (ENSO). A major result is the significant positive trend of ozone in the upper stratosphere, observed at the Jungfraujoch (47°N), which is a typical mid-latitude site, as well as at the high latitude stations. This positive trend in the upper stratosphere at Jungfraujoch provides a sign of ozone recovery at mid-latitudes. [less ▲]

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See detailOzone tropospheric and stratospheric trends (1995-2011) at six ground-based FTIR stations (28°N to 79°N)
Vigouroux, Corinne; De Mazière, Martine; Demoulin, Philippe ULg et al

Poster (2012, August)

Five ground-based stations in Western Europe, from 79°N to 28°N, all part of the Network for the Detection of Atmospheric Composition Change (NDACC), have joined their efforts to homogenize and optimize ... [more ▼]

Five ground-based stations in Western Europe, from 79°N to 28°N, all part of the Network for the Detection of Atmospheric Composition Change (NDACC), have joined their efforts to homogenize and optimize the retrievals of ozone profiles from FTIR (Fourier transform infrared) solar absorption spectra. Using the optimal estimation method, distinct vertical information can be obtained in four layers: ground—10 km, 10—18 km, 18—27 km, and 27—42 km, in addition to total column amounts. Vigouroux et al. (2008) applied a bootstrap resampling method to the ozone data to determine the trends of the total columns and of the partial columns in the above four layers, over the period 1995-2004. The updated trends for the period 1995-2009 have been published in the WMO 2010 report. Here, we present the updated trends, obtained using the bootstrap resampling method, for the 1995-mid-2011 period, for the five European stations and also for the station Thule, Greenland (77°N), which has joined this effort. The trends have also been estimated using a multiple regression model including the Quasi Biennial Oscillation (QBO) and the solar flux as explanatory variables. The trends obtained by the two methods will be compared and discussed. One of the major results is the significant positive trend observed in the upper stratosphere at the station Jungfraujoch (47°N), which provides a sign of ozone recovery at mid-latitudes. Significant positive trends are also observed in the upper stratosphere at the high latitude stations. [less ▲]

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See detailAdvanced exploitation of Ground-Based measurements for Atmospheric Chemistry and Climate Applications "AGACC"
De Mazière, Martine; De Backer, Hugo; Carleer, Michel et al

Report (2011)

We live in an era in which human activities are causing significant changes to the atmospheric environment which result in local to global consequences on the ecosystems. Changes in the atmospheric ... [more ▼]

We live in an era in which human activities are causing significant changes to the atmospheric environment which result in local to global consequences on the ecosystems. Changes in the atmospheric composition impact our climate via chemical and dynamical feedback mechanisms; in many instances they also affect air quality, and the health of the biosphere. Monitoring and understanding those changes and their consequences is fundamental to establish adequate actions for adaptation to and mitigation of the environmental changes. Furthermore, after implementation of regulatory measures like the Montreal Protocol, it is necessary to verify whether the measures are effective. This can only be achieved if we have adequate detection methods and a reliable long record of a series of key geophysical parameters. Thus the AGACC project contributes to the provision of basic new knowledge regarding the atmospheric composition and its changes, based on advanced groundbased monitoring, in combination with satellite and numerical modelling data. Its results are integrated in ongoing international research programmes. The general objective of AGACC has been to improve and extend the groundbased detection capabilities for a number of climate-related target species and, based hereupon, analyse past and present observations to derive new information about the atmospheric composition, its variability and long-term changes. Despite the advent of a growing and more performant fleet of Earth Observation satellites, ground-based observations are still indispensable to (1) guarantee long-term continuity, homogeneity and high quality of the data, and (2) to underpin the satellite data for calibration and (long-term) validation. A first target gas is atmospheric water vapour. It is the key trace gas controlling weather and climate. It is also the most important greenhouse gas in the Earth’s atmosphere. Its amount and vertical distribution are changing, but how and why? Especially in the upper troposphere - lower stratosphere, the radiative effects of changes in the water vapour are significant and should be quantified. The measurement of water vapour is a hot topic since several years. It is a challenge, because water vapour exhibits a large gradient in its concentration when going from the ground to the stratosphere, and because it is highly variable in time and space. For example, we have found that the time scale of the variations of the total water vapour amount at Jungfraujoch is in the order of minutes. In AGACC, we have therefore investigated various experimental techniques to measure the concentration of water vapour in the atmosphere, focusing on the total column as well as on the vertical distribution in the troposphere up to the lower stratosphere. The retrieval of water vapour vertical profiles and total columns from ground-based FTIR data has been initiated at three very different stations where correlative data for verification are available, namely Ukkel (± sea level, mid-latitude), Ile de La Réunion (± sea level, tropical) and Jungfraujoch (high altitude, mid-latitude), with promising results. In particular, at Jungfraujoch, it has been demonstrated that the precision of the FTIR integrated water vapour (IWV) measurements is of order 2%. The capability to retrieve individual isotopologues of water vapour, and to monitor their daily and diurnal variations, has also been demonstrated. This could open new ways to study in the future the role of water vapour in the radiative balance, the global circulation, precipitation etc. We also started joint exploitation of ground-based FTIR and satellite IASI data for water vapour and its isotopologues, in order to exploit fully the potential of the existing instrumentation. A correction method for the radiosoundings at Ukkel has been successfully implemented, resulting in a homogeneous and reliable time series from 1990 to 2008 from which trends in upper troposphere humidity (UTH) and tropopause characteristics have been derived. One observes a rising UTH until September 2001, followed by a decline, accompanied by a descent and heating of the tropopause up to the turning point and an ascent and cooling afterwards. The changes after September 2001 in the upper troposphere can be explained by surface heating and convective uplift. At Jungfraujoch, one does not observe any significant trend in the total water vapour abundance above the station over the 1988-2010 time period, although significant positive summer and negative winter trends have been detected. We have made a quantitative statistical comparison between ground-based FTIR, CIMEL, GPS and integrated (corrected) radio sounding measurements of the IWV at Ukkel. This work is important to better characterize the different sensors in order to exploit together different observations made by different instruments. A second target species is atmospheric aerosol. There is a very large variety of aerosol both from natural or anthropogenic origin. One of the reasons why they are so important is that they affect the optical properties of the atmosphere. In particular, it has been demonstrated in previous studies that the aerosols have a large impact on the quantity of harmful UV-B radiation received at the Earth’s surface. The latest IPCC Report also stressed that the radiative forcing caused by atmospheric aerosols is one of the largest uncertainties in determining the total radiative forcing in the atmosphere. Better monitoring capabilities of aerosol properties can therefore improve our understanding and forecasting of the atmospheric processes and evolution, and in particular of UV-B and climate changes. Several measurement techniques are now operational in the AGACC consortium for the ground-based monitoring of aerosol properties. These are the Brewer spectrometer and CIMEL observations at Ukkel, the latter contributing also to the AERONET network since July 2006, and the newly developed MAXDOAS observations. Unlike CIMEL and Brewer measurements, that provide the total Aerosol Optical Depth, it has been demonstrated that the MAXDOAS measurements also provide additional information about the vertical distribution of the aerosol extinction in the lowest kilometres of the troposphere. A better understanding of the ultimate capabilities of MAXDOAS aerosol remote sensing has been gained through participation to the international CINDI campaign (Cabauw Intercomparison Campaign of Nitrogen Dioxide measuring Instruments ) in summer 2009. The combination of Brewer, CIMEL and MAXDOAS instruments gives us a remote-sensing dataset that will enable a more comprehensive characterization of the tropospheric aerosol optical properties. The usefulness of these aerosol observations has already been demonstrated in the improvement of the UVindex predictions for the general public. Another application is their use as input data in the retrieval of vertical profiles of tropospheric pollutants from MAXDOAS measurements, like tropospheric NO2 and formaldehyde. Third we have focused on a few climate-related trace gases. Changing greenhouse gas and aerosol concentrations directly affect the radiative budget of the atmosphere, and therefore climate. But many species known as pollutants like carbon monoxide (CO), nitrogen oxides (NOx) and hydrocarbons, - often related to fossil fuel or biomass burning -, also affect climate through their role in chemical reactions that produce tropospheric ozone, which is a well-known greenhouse gas, or that modify the lifetime of gases like methane, or the oxidation capacity of the atmosphere. Therefore in AGACC, we have focused on the measurement of a number of trace gases that are subject to changing concentrations, that directly or indirectly affect climate, and that are either difficult to monitor or that have not yet been measured from the ground. We have included attempts to observe distinctly some isotopologues, because the isotopic ratios observed in an airmass provide information on its history, and because the FTIR solar absorption measurements provide a rather unique capability hereto. The investigated species are the isotopologues of CH4 and CO, and hydrogen cyanide (HCN), as examples of biomass burning tracers, some hydrocarbons like formaldehyde (HCHO), ethylene (C2H4) and acetylene (C2H2), and HCFC-142b, a replacement product for CFCs and a greenhouse gas. In many cases, retrieval strategies had to be adapted when going from one site to another with different atmospheric conditions, especially when the local humidity and abundances are very different as is the case between Jungfraujoch (dry, high altitude, mid-latitude) and Ile de La Réunion (humid, low altitude, low latitude). Still we have been able to show the feasibility of retrieving particular trace gas information even under difficult conditions. Many of our results have been compared to correlative data, to validate the approach and to gain complementary information. It is also important to note that the retrieval strategies developed in AGACC have regularly been presented to the global Network for the Detection of Atmospheric Composition Change (NDACC) UV-Vis and Infrared communities and have often been adopted by others or even proposed for adoption as a standard in the community (e.g., for hydrogen cyanide (HCN)). In particular: We have been able to study the seasonal variations of HCN at the Jungfraujoch and at Ile de La Réunion, and to show the dominant impact of biomass burning. Formaldehyde was studied in much detail at Ukkel, Jungfraujoch and Ile de la Réunion. The challenge for detection at Jungfraujoch is the small abundance (about 10 times smaller than at Ukkel and Ile de La Réunion); a particular observation strategy was developed successfully, resulting in a time series that already shows the day-to-day and seasonal variations. At Ile de La Réunion, comparisons of FTIR, MAXDOAS, satellite and model data have (1) shown the good agreement between the various data sets, but also, (2), the variability of HCHO (diurnal, seasonal, day-to-day), and (3), thanks to the complementarities of the various data sets, they have enabled us to learn more about the long-range transport of Non-methane Volatile Organic Compounds (NMVOCS, precursors of HCHO) and deficiencies in the models. It was shown that fast, direct transport of NMVOCS from Madagascar has a significant impact on the HCHO abundance and its variability at Ile de La Réunion, and that this is underestimated in the model. Significant progress was made as to the detection of 13CH4 and CH3D from ground-based FTIR observations, both at Jungfraujoch and Ile de La Réunion. To our knowledge, it is the first time that a d13C data set is derived from ground-based FTIR observations. More work is needed to improve the CH3D retrieval at Ile de La Réunion, and to interpret the results, in combination with models. Also for the first time, 12CO and 13CO have been retrieved individually at Jungfraujoch. The d13C time series shows significant seasonal and interannual changes. As to the hydrocarbon ethylene, it is shown that it can be detected at Jungfraujoch only in spectra at low solar elevation, given its small atmospheric abundance. Regarding acetylene, the observed time series at Jungfraujoch and Ile de La Réunion show clear seasonal variations and enhancements due to the impact of biomass burning events, correlated with enhancements in CO, C2H6 and HCN. It is not clear yet whether we can reliably retrieve the concentration of HCFC- 142b, a replacement product that is increasing strongly in the troposphere. New line parameters for the interfering species HFC-134a are required to confirm/infirm the preliminary results. This highlights again the importance of the laboratory work for providing such parameters. Improved line parameters have been obtained for water vapour and its isotopologues, ethylene and formic acid. These AGACC results have been integrated in the international spectroscopic databases. We also showed that line intensities available around 2096 cm–1 for the 13C16O isotopologue of carbon monoxide in the HITRAN database seem to be accurate to 2%. We failed to improve line intensities for the 13.6 μm region of acetylene. The new data sets that have been derived in AGACC from FTIR and MAXDOAS observations have been archived in the NDACC data centre, where they are available for users (generally modelers and satellite teams). In addition, they are stored locally and are available to users upon request. AGACC results have been reported to the international scientific community, via the literature, via integration in geophysical or spectroscopic databases, and via participation to international research initiatives like the Atmospheric Water Vapour in the Climate System (WAVACS) Cost Action, the International Space Science Institute (ISSI) Working Group on Atmospheric Water Vapour, the International Union of Pure and Applied Chemistry (IUPAC) project, the International CINDI campaign, etc. The results have already found important scientific applications. A few examples are worth mentioning: the re-evaluation of methane emissions in the tropics from SCIAMACHY based on the new H2O spectroscopy, and the improved retrievals of HCOOH from the satellite experiments ACE-FTS and IASI, and from the ground. In the longer-term, the AGACC results will no doubt benefit the research in atmospheric sciences –in particular in the monitoring of its composition changes–, which is the fundamental basis of environmental assessment reports for supporting policy makers. [less ▲]

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See detailFirst retrievals of methyl chloride from ground-based high-resolution FTIR solar observations
Mahieu, Emmanuel ULg; Harrison, Jeremy; Bernath, Peter F. et al

in Geophysical Research Abstracts (2011), 13

Methyl chloride (CH3Cl) is one of the most abundant chlorine-bearing gas in the Earth’s troposphere and a significant contributor to the organic chlorine budget. Measurements by in situ networks indicate ... [more ▼]

Methyl chloride (CH3Cl) is one of the most abundant chlorine-bearing gas in the Earth’s troposphere and a significant contributor to the organic chlorine budget. Measurements by in situ networks indicate a mean volume mixing ratio of 550 pptv, with a significant seasonal cycle of about 80 pptv, peak to peak. This species also exhibits inter-annual variability, but no long-term trend. Major sources are from tropical and sub-tropical plants and dead leaves, the oceans and biomass burning. Some industrial processes and waste incineration further add to the emissions. Oxidation by the hydroxyl radical is by far the largest CH3Cl sink, followed by soil uptake. Although balanced, its atmospheric budget is still affected by large uncertainties and contributions from unidentified sources and sinks cannot be ruled out. Methyl chloride has an atmospheric lifetime of 1 year, a global warming potential of 13 (100-yr horizon) and an ozone depleting potential of 0.02. The retrieval of methyl chloride from ground-based infrared (IR) spectra is very challenging. Indeed, numerous interferences by strong water vapor and methane lines complicate the detection of small CH3Cl absorptions, close to 1%, near 3 microns. In addition, and although weak, ethane features contribute to the difficulty, in particular since a significant number of ethane branches were absent until very recently from official HITRAN compilations. Therefore, the scientific literature does not report thus far about any investigations of CH3Cl from ground-based remote sensing observations. In this contribution, we will present first CH3Cl total column retrievals, using the SFIT-2 algorithm (v3.94) and high-resolution Fourier Transform Infrared (FTIR) solar absorption observations recorded with a 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). In our retrievals, we use new ethane absorption cross sections recorded at the Molecular Spectroscopy Facility of the Rutherford Appleton Laboratory (Harrison et al., 2010). They were calibrated in intensity by using reference low-resolution spectra from the Pacific Northwest National Laboratory (PNNL) IR database. These new cross sections were recently released as a HITRAN update (see http://www.hitran.com). 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, including our target CH3Cl. We will evaluate the improvement brought by the new ethane line parameters on the fitting residuals, and characterize the quality, the precision and the reliability of the retrieved product. If successful, a long-term CH3Cl total column time series will be produced using the Jungfraujoch observational database, and we will perform preliminary investigations of the seasonal and inter-annual variations of methyl chloride total columns at northern mid-latitudes. [less ▲]

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See detailRecent trends of inorganic chlorine and halogenated source gases above the Jungfraujoch and Kitt Peak stations derived from high-resolution FTIR solar observations
Mahieu, Emmanuel ULg; Rinsland, Curtis P.; Gardiner, Tom et al

in Geophysical Research Abstracts (2010), 12(EGU2010-2420-3),

The longest series of Fourier Transform Infrared (FTIR) high spectral resolution solar absorption observations are available from the Jungfraujoch and Kitt Peak stations, located at 46.5ºN and 30.9ºN ... [more ▼]

The longest series of Fourier Transform Infrared (FTIR) high spectral resolution solar absorption observations are available from the Jungfraujoch and Kitt Peak stations, located at 46.5ºN and 30.9ºN, respectively. State-of-the-art interferometers are operated at these sites within the framework of the Network for the Detection of Atmospheric Composition Change (NDACC, visit http://www.ndacc.org). These instruments allow to record spectra on a regular basis, under clear-sky conditions, using a suite of optical filters which altogether cover the 2 to 16 micron spectral range. Numerous absorption features characterized in the HITRAN compilations (e.g. Rothman et al., 2008) are encompassed in this mid-infrared region. Their analyses with either the SFIT-1 or SFIT-2 algorithm allow retrieving total columns of the target gases. Moreover, information on their distribution with altitude can generally be derived when using SFIT-2 which implements the Optimal Estimation Method of Rodgers (1990). Among the two dozen gases of atmospheric interest accessible to the ground-based FTIR technique, we have selected here a suite of long-lived halogenated species: HCl, ClONO2, CCl2F2, CCl3F, CHClF2, CCl4 and SF6. Time series available from the two sites will be presented, compared and critically discussed. In particular, changes in the abundances of theses gases since the peak in inorganic chlorine (Cly, which occurred in 1996-1997) and their intra-annual variability will be characterized with a statistical tool using bootstrap resampling (Gardiner et al., 2008). Trends and their associated uncertainties will be reported and put into perspective with the phase-out regulations of the production of ozone depleting substances adopted and implemented by the Montreal Protocol, its Amendments and Adjustments. For instance, the trends affecting the reservoir species HCl, ClONO2, and their summation which is a good proxy of the total inorganic chlorine, have been calculated using all available daily mean measurements from January 1996 onwards. The following values were obtained for Jungfraujoch, when using 1996 as the reference year: -0.90±0.10%/yr for HCl, -0.92±0.26 %/yr for ClONO2, and -0.96±0.14 %/yr for Cly; in all cases, the uncertainties define the 95% confidence interval around the trend values. For Kitt Peak, the corresponding trends are: -0.55±0.34 %/yr for HCl, -1.27±0.84 %/yr for ClONO2 and -0.61±0.51 %/yr for Cly, they are statistically consistent with the Jungfraujoch rates of decrease. Further trend data will be presented at the EGU General Assembly while supplementary information on Jungfraujoch results will be available from communications at the same meeting by Duchatelet et al. (2010), Lejeune et al (2010) and Rinsland et al (2010). Comparisons with model data are also foreseen. [less ▲]

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See detailDetermination of isotopic fractionation delta13C of methane from ground-based FTIR observations performed at the Jungfraujoch
Duchatelet, Pierre ULg; Mahieu, Emmanuel ULg; Sussmann, Ralf et al

Poster (2009, April)

Atmospheric methane (CH4) is a strong greenhouse gas that has important chemical impacts on both the troposphere and the stratosphere. In the troposphere, oxidation of methane is a major regulator of OH ... [more ▼]

Atmospheric methane (CH4) is a strong greenhouse gas that has important chemical impacts on both the troposphere and the stratosphere. In the troposphere, oxidation of methane is a major regulator of OH and is a source of formaldehyde, carbon monoxide and hydrogen. In the stratosphere, CH4 plays a central role (i), due to its contribution to the stratospheric water vapor budget, and (ii), as a sink for chlorine atoms which reduces the rate of stratospheric ozone depletion. Because the different sources of methane (natural and anthropogenic like wetlands, rice paddies, termites, natural gas escape, biomass burning, etc) have distinct 13C/12C ratios (usually reported in “delta” notation δ13C), measurements of atmospheric 13CH4 content, in addition to those of the main isotopologue (12CH4), can be used to investigate individual source strengths as well as their spatial and temporal distributions. Characterization of the isotopic fractionation of methane is therefore important, for example, to help models constrain estimates of the global methane budget. However, experimental data for the 13C/12C isotope ratio are sparse. The currently accepted average value of δ13C in atmospheric methane is about -47‰ (Platt et al., 2004). The first goal of this work is to develop and to characterize (in terms of information content and error budget) an original retrieval approach to derive 13CH4 columns from ground-based Fourier transform infrared (FTIR) spectra recorded at the International Scientific Station of the Jungfraujoch (ISSJ; 46.5°N, 8.0°E, 3580m a.s.l., Swiss Alps). The retrieval strategy is based on a Tikhonov L1 approach which has been originally developed for 12CH4 by Sussmann et al. (2008) [see also contributions by Sussmann et al. to this conference (EGU2009-7869)]. In order to validate our 13CH4 products, comparisons with satellite ACE-FTS (Atmospheric Chemistry Experiment - Fourier Transform Spectrometer) measurements are performed. Then, atmospheric δ13C ratios derived from the FTIR measurements will be compared to values published in the literature and critically discussed. References: Platt, U., W. Allan and D. Lowe, Hemispheric average Cl atom concentration from 13C/12C ratios in atmospheric methane, Atmos. Chem. Phys., 4, 2393-2399, 2004. Sussmann, R., Forster, F., Borsdorff, T., et al.: Satellite validation of column-averaged methane on global scale: ground-based data from 15 FTIR stations versus last generation ENVISAT/SCIAMACHY retrievals, IGAC 10th International Conference, Annecy, France, 7-12 Sep 2008. [less ▲]

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See detailGround-based CO observations at the Jungfraujoch from 1997 till 2007: Comparison between FTIR and NDIR measurements
Dils, Bart; Demoulin, Philippe ULg; Mahieu, Emmanuel ULg et al

Poster (2009, January 26)

Here we will discuss CO measurements taken at the Swiss Alpine Jungfraujoch station (46.5º N, 8.0° E, 3580m a.s.l.) over the 1997-2007 time period. Results from two distinct techniques, namely Fourier ... [more ▼]

Here we will discuss CO measurements taken at the Swiss Alpine Jungfraujoch station (46.5º N, 8.0° E, 3580m a.s.l.) over the 1997-2007 time period. Results from two distinct techniques, namely Fourier Transform Infrared solar absorption spectrometry (FTIR), and the in situ Nondispersive Infrared technique (NDIR) have been compared. While the in situ NDIR measurements detect local CO concentrations at the site, the FTIR technique provides integrated measurements along the line-of-sight. Nevertheless, the pressure broadening of the spectral absorption lines recorded at high resolution enables retrieving information on the vertical distribution of CO, mainly in the troposphere, including its concentration near the surface. To provide enough information content the averaged vmr between 3.58 and 7 km is derived from the FTIR profile data. Both datasets show a significant negative trend over the time period. However, the NDIR dataset's negative trend is much stronger. Pettitt change point tests reveal that the NDIR-FTIR bias changes substantially from 1997 till 2004 after which the bias stabilizes. Possible causes for these observations will be critically discussed. [less ▲]

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Peer Reviewed
See detailTrend analysis of greenhouse gases over Europe measured by a network of ground-based remote FTIR instruments
Gardiner, Tom; Forbes, A.; De Mazière, Martine et al

in Atmospheric Chemistry and Physics (2008), 8(22), 6719-6727

This paper describes the statistical analysis of annual trends in long term datasets of greenhouse gas measurements taken over ten or more years. The analysis technique employs a bootstrap resampling ... [more ▼]

This paper describes the statistical analysis of annual trends in long term datasets of greenhouse gas measurements taken over ten or more years. The analysis technique employs a bootstrap resampling method to determine both the long-term and intra-annual variability of the datasets, together with the uncertainties on the trend values. The method has been applied to data from a European network of ground-based solar FTIR instruments to determine the trends in the tropospheric, stratospheric and total columns of ozone, nitrous oxide, carbon monoxide, methane, ethane and HCFC-22. The suitability of the method has been demonstrated through statistical validation of the technique, and comparison with ground-based in-situ measurements and 3-D atmospheric models. [less ▲]

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See detailValidation of ACE-FTS v2.2 measurements of HCl, HF, CCl3F and CCl2F2 using space-, balloon- and ground-based instrument observations
Mahieu, Emmanuel ULg; Duchatelet, Pierre ULg; Demoulin, Philippe ULg et al

in Atmospheric Chemistry and Physics (2008), 8

Hydrogen chloride (HCl) and hydrogen fluoride (HF) are respectively the main chlorine and fluorine reservoirs in the Earth's stratosphere. Their buildup resulted from the intensive use of man-made ... [more ▼]

Hydrogen chloride (HCl) and hydrogen fluoride (HF) are respectively the main chlorine and fluorine reservoirs in the Earth's stratosphere. Their buildup resulted from the intensive use of man-made halogenated source gases, in particular CFC-11 (CCl3F) and CFC-12 (CCl2F2), during the second half of the 20th century. It is important to continue monitoring the evolution of these source gases and reservoirs, in support of the Montreal Protocol and also indirectly of the Kyoto Protocol. The Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) is a space-based instrument that has been performing regular solar occultation measurements of over 30 atmospheric gases since early 2004. In this validation paper, the HCl, HF, CFC-11 and CFC-12 version 2.2 profile data products retrieved from ACE-FTS measurements are evaluated. Volume mixing ratio profiles have been compared to observations made from space by MLS and HALOE, and from stratospheric balloons by SPIRALE, FIRS-2 and Mark-IV. Partial columns derived from the ACE-FTS data were also compared to column measurements from ground-based Fourier transform instruments operated at 12 sites. ACE-FTS data recorded from March 2004 to August 2007 have been used for the comparisons. These data are representative of a variety of atmospheric and chemical situations, with sounded air masses extending from the winter vortex to summer sub-tropical conditions. Typically, the ACE-FTS products are available in the 10-50 km altitude range for HCl and HF, and in the 7-20 and 7-25 km ranges for CFC-11 and -12, respectively. For both reservoirs, comparison results indicate an agreement generally better than 5-10% above 20 km altitude, when accounting for the known offset affecting HALOE measurements of HCl and HF. Larger positive differences are however found for comparisons with single profiles from FIRS-2 and SPIRALE. For CFCs, the few coincident measurements available suggest that the differences probably remain within +/-20%. [less ▲]

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See detailValidation of SCIAMACHY CH4 scientific products using ground-based FTIR measurements
Dils, Bart; De Mazière, Martine; Vigouroux, Corinne et al

Poster (2008, September)

In the framework of the past EVERGREEN project, the development of three scientific algorithms, namely WFM-DOAS (henceforward called WFMD), IMAP-DOAS (henceforward called IMAP) and IMLM, commenced in ... [more ▼]

In the framework of the past EVERGREEN project, the development of three scientific algorithms, namely WFM-DOAS (henceforward called WFMD), IMAP-DOAS (henceforward called IMAP) and IMLM, commenced in order to retrieve the total column amounts of key atmospheric trace gases, including CH4, from SCIAMACHY nadir observations in its near-infrared channels. Since then, the retrieval products of these three algorithms, have undergone serious improvements. At key phases in their development, the products have been validated by using a network of ground-based FTIR instruments. Parallel with the improved SCIAMACHY data, the FTIR groups have taken steps to optimise and harmonise their own datasets and as such the different validation efforts always used the state-of-the-art FTIR dataset. Here we present an overview of the evolution of the CH4 algorithms by re-validating the data, using the same FTIR dataset (as developed under the UFTIR project) for all algorithm versions. [less ▲]

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See detailSatellite validation of column-averaged methane on global scale: ground-based data from 15 FTIR stations versus last generation ENVISAT/SCIAMACHY retrievals
Sussmann, Ralf; Foster, Frank; Borsdorff, Tobias et al

Poster (2008, September)

Previous work has shown that the precision of ground-based mid-infrared (MIR) FTIR spectrometry is sufficient to detect day-to-day variability of columnar methane, while first retrievals from ENVISAT ... [more ▼]

Previous work has shown that the precision of ground-based mid-infrared (MIR) FTIR spectrometry is sufficient to detect day-to-day variability of columnar methane, while first retrievals from ENVISAT/SCIAMACHY (channel 8) satellite measurements were impacted by a significant time-dependent bias due to detector icing. This prevented insight into true methane temporal variability at that time. The goal of our updated study is to investigate the precision of the last generation (channel 6) SCIAMACHY retrievals IMAP-DOAS v49 and WFM-DOAS v1.0 in comparison to retrievals from ground-based MIR measurements of the European FTIR network. We first briefly discuss the origin and magnitude of the natural variability of columnar methane. Subsequently, our study investigates all factors which can be optimized to improve precision of ground-based MIR-FTIR retrievals of columnar methane. This includes an optimized Tikhonov-type regularization tuned in a way to minimize the diurnal variability of retrieved columnar methane. We also discuss ways to select and average individual-pixel satellite data in order to reflect true day-to-day variability and make them comparable to ground-based data. [less ▲]

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See detailValidation of ACE-FTS N2O measurements
Strong, Kimberley; Wolff, Mareile A; Kerzenmacher, Tobias E et al

in Atmospheric Chemistry and Physics (2008), 8(16), 4759-4786

The Atmospheric Chemistry Experiment (ACE), also known as SCISAT, was launched on 12 August 2003, carrying two instruments that measure vertical profiles of atmospheric constituents using the solar ... [more ▼]

The Atmospheric Chemistry Experiment (ACE), also known as SCISAT, was launched on 12 August 2003, carrying two instruments that measure vertical profiles of atmospheric constituents using the solar occultation technique. One of these instruments, the ACE Fourier Transform Spectrometer (ACE-FTS), is measuring volume mixing ratio (VMR) profiles of nitrous oxide (N2O) from the upper troposphere to the lower mesosphere at a vertical resolution of about 3-4 km. In this study, the quality of the ACE-FTS version 2.2 N2O data is assessed through comparisons with coincident measurements made by other satellite, balloon-borne, aircraft, and ground-based instruments. These consist of vertical profile comparisons with the SMR, MLS, and MIPAS satellite instruments, multiple aircraft flights of ASUR, and single balloon flights of SPIRALE and FIRS-2, and partial column comparisons with a network of ground-based Fourier Transform InfraRed spectrometers (FTIRs). Between 6 and 30 km, the mean absolute differences for the satellite comparisons lie between -42 ppbv and +17 ppbv, with most within +/- 20 ppbv. This corresponds to relative deviations from the mean that are within +/- 15%, except for comparisons with MIPAS near 30 km, for which they are as large as 22.5%. Between 18 and 30 km, the mean absolute differences for the satellite comparisons are generally within +/- 10 ppbv. From 30 to 60 km, the mean absolute differences are within +/- 4 ppbv, and are mostly between -2 and +1 ppbv. Given the small N2O VMR in this region, the relative deviations from the mean are therefore large at these altitudes, with most suggesting a negative bias in the ACE-FTS data between 30 and 50 km. In the comparisons with the FTIRs, the mean relative differences between the ACE-FTS and FTIR partial columns (which cover a mean altitude range of 14 to 27 km) are within +/- 5.6% for eleven of the twelve contributing stations. This mean relative difference is negative at ten stations, suggesting a small negative bias in the ACE-FTS partial columns over the altitude regions compared. Excellent correlation (R=0.964) is observed between the ACE-FTS and FTIR partial columns, with a slope of 1.01 and an intercept of -0.20 on the line fitted to the data. [less ▲]

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See detailImpact of different spectroscopic datasets on CH4 retrievals from Jungfraujoch FTIR spectra
Duchatelet, Pierre ULg; Mahieu, Emmanuel ULg; Demoulin, Philippe ULg et al

Poster (2008, August)

Methane (CH4) is released in the atmosphere by natural processes (e.g. wetlands, termites) as well as by anthropogenic activities (e.g. fossil fuel exploitation, rice agriculture, biomass burning, etc ... [more ▼]

Methane (CH4) is released in the atmosphere by natural processes (e.g. wetlands, termites) as well as by anthropogenic activities (e.g. fossil fuel exploitation, rice agriculture, biomass burning, etc). Due to its high warming potential and its relatively long chemical lifetime (~9 years), atmospheric methane plays a major role in the radiative forcing responsible of the greenhouse effect. Methane also affects climate by influencing tropospheric ozone and stratospheric water. The cycle of methane is complex and to understand it requires a complete study of its emissions and its budget of sources and sinks. High quality methane data sets are needed to perform such studies. CH4 vertical distributions as well as total and partial column time series can be retrieved from high-resolution ground-based FTIR spectra, using, e.g., the SFIT-2 algorithm which implements the Optimal Estimation Method of Rodgers. A set of 5 microwindows - located in the 2 to 5.5 µm range and jointly adopted by all partners involved in the European HYMN project (www.knmi.nl/samenw/hymn/) - are fitted simultaneously during the retrieval procedure. Although this approach provides relatively high information content, CH4 retrieved profiles very often present large oscillations in the troposphere, which might result partly from inappropriate or inconsistent spectroscopic parameters. Significant improvements on retrieval quality could be reached by using more accurate CH4 spectroscopic parameters. This contribution compares 3 different sets of CH4 spectroscopic parameters (including HITRAN 2004 and 2 versions where HITRAN 2004 have been updated by recent laboratory measurements), which have been tested using one year of high resolution FTIR solar observations performed at the International Scientific Station of the Jungfraujoch (Swiss Alps, 46.5°N, 8.0 °E, 3580m a.s.l.). The impact of these different spectroscopic datasets on retrieved CH4 partial columns and vertical profiles, as well as on the fitting quality (residuals) and on the error budget characterizing our CH4 products will be evaluated and discussed. [less ▲]

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See detailValidation of HNO3, ClONO2, and N2O5 from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS)
Wolff, Mareile; Kerzenmacher, Tobias; Strong, Kimberley et al

in Atmospheric Chemistry and Physics (2008), 8(13), 3529-3562

The Atmospheric Chemistry Experiment (ACE) satellite was launched on 12 August 2003. Its two instruments measure vertical profiles of over 30 atmospheric trace gases by analyzing solar occultation spectra ... [more ▼]

The Atmospheric Chemistry Experiment (ACE) satellite was launched on 12 August 2003. Its two instruments measure vertical profiles of over 30 atmospheric trace gases by analyzing solar occultation spectra in the ultraviolet/visible and infrared wavelength regions. The reservoir gases HNO3, ClONO2, and N2O5 are three of the key species provided by the primary instrument, the ACE Fourier Transform Spectrometer (ACE-FTS). This paper describes the ACE-FTS version 2.2 data products, including the N2O5 update, for the three species and presents validation comparisons with available observations. We have compared volume mixing ratio (VMR) profiles of HNO3, ClONO2, and N2O5 with measurements by other satellite instruments (SMR, MLS, MIPAS), aircraft measurements (ASUR), and single balloon-flights (SPIRALE, FIRS-2). Partial columns of HNO3 and ClONO2 were also compared with measurements by ground-based Fourier Transform Infrared (FTIR) spectrometers. Overall the quality of the ACE-FTS v2.2 HNO3 VMR profiles is good from 18 to 35 km. For the statistical satellite comparisons, the mean absolute differences are generally within ±1 ppbv ±20%) from 18 to 35 km. For MIPAS and MLS comparisons only, mean relative differences lie within±10% between 10 and 36 km. ACE-FTS HNO3 partial columns (~15–30 km) show a slight negative bias of −1.3% relative to the ground-based FTIRs at latitudes ranging from 77.8° S–76.5° N. Good agreement between ACE-FTS ClONO2 and MIPAS, using the Institut für Meteorologie und Klimaforschung and Instituto de Astrofísica de Andalucía (IMK-IAA) data processor is seen. Mean absolute differences are typically within ±0.01 ppbv between 16 and 27 km and less than +0.09 ppbv between 27 and 34 km. The ClONO2 partial column comparisons show varying degrees of agreement, depending on the location and the quality of the FTIR measurements. Good agreement was found for the comparisons with the midlatitude Jungfraujoch partial columns for which the mean relative difference is 4.7%. ACE-FTS N2O5 has a low bias relative to MIPAS IMK-IAA, reaching −0.25 ppbv at the altitude of the N2O5 maximum (around 30 km). Mean absolute differences at lower altitudes (16–27 km) are typically −0.05 ppbv for MIPAS nighttime and ±0.02 ppbv for MIPAS daytime measurements. [less ▲]

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See detailTechnical Note: New ground-based FTIR measurements at Ile de La Réunion: observations, error analysis, and comparisons with independent data
Senten, Cindy; De Mazière, Martine; Dils, Bart et al

in Atmospheric Chemistry and Physics (2008), 8(13), 3483-3508

Ground-based high spectral resolution Fourier-transform infrared (FTIR) solar absorption spectroscopy is a powerful remote sensing technique to obtain information on the total column abundances and on the ... [more ▼]

Ground-based high spectral resolution Fourier-transform infrared (FTIR) solar absorption spectroscopy is a powerful remote sensing technique to obtain information on the total column abundances and on the vertical distribution of various constituents in the atmosphere. This work presents results from two FTIR measurement campaigns in 2002 and 2004, held at Ile de La Réunion (21° S, 55° E). These campaigns represent the first FTIR observations carried out at a southern (sub)tropical site. They serve the initiation of regular, long-term FTIR monitoring at this site in the near future. To demonstrate the capabilities of the FTIR measurements at this location for tropospheric and stratospheric monitoring, a detailed report is given on the retrieval strategy, information content and corresponding full error budget evaluation for ozone (O3), methane (CH4), nitrous oxide (N2O), carbon monoxide (CO), ethane (C2H6), hydrogen chloride (HCl), hydrogen fluoride (HF) and nitric acid (HNO3) total and partial column retrievals. Moreover, we have made a thorough comparison of the capabilities at sea level altitude (St.-Denis) and at 2200 m a.s.l. (Maïdo). It is proved that the performances of the technique are such that the atmospheric variability can be observed, at both locations and in distinct altitude layers. Comparisons with literature and with correlative data from ozone sonde and satellite (i.e., ACE-FTS, HALOE and MOPITT) measurements are given to confirm the results. Despite the short time series available at present, we have been able to detect the seasonal variation of CO in the biomass burning season, as well as the impact of particular biomass burning events in Africa and Madagascar on the atmospheric composition above Ile de La Réunion. We also show that differential measurements between St.-Denis and Maïdo provide useful information about the concentrations in the boundary layer. [less ▲]

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See detailCO measurements from the ACE-FTS satellite instrument: data analysis and validation using ground-based, airborne and spaceborne observations
Clerbaux, Catherine; George, Maya; Turquety, Solène et al

in Atmospheric Chemistry and Physics (2008), 8

The Atmospheric Chemistry Experiment (ACE) mission was launched in August 2003 to sound the atmosphere by solar occultation. Carbon monoxide (CO), a good tracer of pollution plumes and atmospheric ... [more ▼]

The Atmospheric Chemistry Experiment (ACE) mission was launched in August 2003 to sound the atmosphere by solar occultation. Carbon monoxide (CO), a good tracer of pollution plumes and atmospheric dynamics, is one of the key species provided by the primary instrument, the ACE-Fourier Transform Spectrometer (ACE-FTS). This instrument performs measurements in both the CO 1-0 and 2-0 ro-vibrational bands, from which vertically resolved CO concentration profiles are retrieved, from the mid-troposphere to the thermosphere. This paper presents an updated description of the ACE-FTS version 2.2 CO data product, along with a comprehensive validation of these profiles using available observations (February 2004 to December 2006). We have compared the CO partial columns with ground-based measurements using Fourier transform infrared spectroscopy and millimeter wave radiometry, and the volume mixing ratio profiles with airborne (both high-altitude balloon flight and airplane) observations. CO satellite observations provided by nadir-looking instruments (MOPITT and TES) as well as limb-viewing remote sensors (MIPAS, SMR and MLS) were also compared with the ACE-FTS CO products. We show that the ACE-FTS measurements provide CO profiles with small retrieval errors (better than 5% from the upper troposphere to 40 km, and better than 10% above). These observations agree well with the correlative measurements, considering the rather loose coincidence criteria in some cases. Based on the validation exercise we assess the following uncertainties to the ACE-FTS measurement data: better than 15% in the upper troposphere (8–12 km), than 30% in the lower stratosphere (12–30 km), and than 25% from 30 to 100 km. [less ▲]

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See detailValidation of ACE-FTS v2.2 methane profiles from the upper troposphere to the lower mesosphere
De Mazière, Martine; Vigouroux, Corinne; Bernath, Peter et al

in Atmospheric Chemistry and Physics (2008), 9(9), 2421-2435

The ACE-FTS (Atmospheric Chemistry Experiment – Fourier Transform Spectrometer) solar occultation instrument that was launched onboard the Canadian SCISAT-1 satellite in August 2003 is measuring vertical ... [more ▼]

The ACE-FTS (Atmospheric Chemistry Experiment – Fourier Transform Spectrometer) solar occultation instrument that was launched onboard the Canadian SCISAT-1 satellite in August 2003 is measuring vertical profiles from the upper troposphere to the lower mesosphere for a large number of atmospheric constituents. Methane is one of the key species. The version v2.2 data of the ACE-FTS CH4 data have been compared to correlative satellite, balloon-borne and ground-based Fourier transform infrared remote sensing data to assess their quality. The comparison results indicate that the accuracy of the data is within 10% in the upper troposphere – lower stratosphere, and within 25% in the middle and higher stratosphere up to the lower mesosphere (<60 km). The observed differences are generally consistent with reported systematic uncertainties. ACE-FTS is also shown to reproduce the variability of methane in the stratosphere and lower mesosphere. [less ▲]

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