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See detailINVESTIGATING MODEL DEFICIENCIES IN THE GLOBAL BUDGET OF ETHANE
Tzompa-Sosa, Z. A.; Keller, C. A.; Turner, A. J. et al

Poster (2015, December 14)

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See detailNonparametric estimation and bootstrap inference on recent trends in atmospheric ethane
Friedrich, Marina; Reuvers, H.; Smeekes, S. et al

Conference (2015, December 12)

Ethane is the most abundant non-methane hydrocarbon in the Earth's atmosphere and an important precursor of tropospheric ozone. Its monitoring is therefore crucial for the characterization of air quality ... [more ▼]

Ethane is the most abundant non-methane hydrocarbon in the Earth's atmosphere and an important precursor of tropospheric ozone. Its monitoring is therefore crucial for the characterization of air quality and of the transport of tropospheric pollution. Ethane is also an indirect greenhouse gas, influencing the atmospheric lifetime of methane. The main sources of ethane are located in the northern hemisphere, and the dominating emissions are associated to production and transport of natural gas. A preliminary trend analysis was conducted using measurements performed in the Swiss Alps. Over the last two decades, the trend of ethane showed a decline of around 1% per year, thanks to a reduction of fugitive emissions of fossil fuel sources. However, a recent upturn potentially attributed to the massive exploitation of shale gas and tight oil reservoirs in North America was found. The goal is to investigate the presence and form of changes in trend functions using nonparametric techniques. The possible location of such changes is investigated. In addition, nonparametric estimation techniques are used to allow for nonlinear trend functions. Given the nonstandard nature of the measurements we rely on dependent wild bootstrap techniques to conduct inference on possible breaks in linear trends and on nonparametric trend functions. [less ▲]

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See detailRetrieval of ammonia from ground-based FTIR solar spectra
Dammers, Enrico; Vigouroux, C; Palm, M et al

in Atmospheric Chemistry and Physics (2015), 15

We present a retrieval method for ammonia (NH3) total columns from ground-based Fourier Transform InfraRed (FTIR) observations. Observations from Bremen (53.10° N, 8.85° E), Lauder (45.04° S, 169.68° E ... [more ▼]

We present a retrieval method for ammonia (NH3) total columns from ground-based Fourier Transform InfraRed (FTIR) observations. Observations from Bremen (53.10° N, 8.85° E), Lauder (45.04° S, 169.68° E), Reunion (20.9° S, 55.50° E) and Jungfraujoch (46.55° N, 7.98° E) were used to illustrate the capabilities of the method. NH3 mean total columns ranging three orders of magnitude were obtained with higher values at Bremen (mean of 13.47 × 1015 molecules cm-2) to the lower values at Jungfraujoch (mean of 0.18 × 1015 molecules cm-2). In conditions with high surface concentrations of ammonia, as in Bremen, it is possible to retrieve information on the vertical gradient as two layers can be discriminated. The retrieval there is most sensitive to ammonia in the planetary boundary layer, where the trace gas concentration is highest. For conditions with low concentrations only the total column can be retrieved. Combining the systematic and random errors we have a mean total error of 26 % for all spectra measured at Bremen (Number of spectra (N) = 554), 30 % for all spectra from Lauder (N =2412), 25 % for spectra from Reunion (N =1262) and 34 % for spectra measured at Jungfraujoch (N =2702). The error is dominated by the systematic uncertainties in the spectroscopy parameters. Station specific seasonal cycles were found to be consistent with known seasonal cycles of the dominant ammonia sources in the station surroundings. The developed retrieval methodology from FTIR-instruments provides a new way to obtain highly time-resolved measurements of ammonia burdens. FTIR-NH3 observations will be useful for understanding the dynamics of ammonia concentrations in the atmosphere and for satellite and model validation. It will also provide additional information to constrain the global ammonia budget. [less ▲]

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See detailDecrease of carbon tetrachloride (CCl4) over 2004-2013 as inferred from global occultation measurements with ACE-FTS
Mahieu, Emmanuel ULg; Bernath, P. F.; Boone, C. D. et al

Poster (2015, October 05)

In this contribution, we use infrared solar occultation measurements performed by the ACE-FTS (Atmospheric Chemistry Experiment – Fourier Transform Spectrometer) instrument onboard the SCISAT-1 Canadian ... [more ▼]

In this contribution, we use infrared solar occultation measurements performed by the ACE-FTS (Atmospheric Chemistry Experiment – Fourier Transform Spectrometer) instrument onboard the SCISAT-1 Canadian satellite (Bernath et al., 2005). Since its launch in August 2003, this spectrometer has been in continuous operation with no significant degradation of its performance, and global measurements are available from late February 2004 onwards, spanning now more than a decade. [less ▲]

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See detailCurrent trend in carbon tetrachloride from several NDACC FTIR stations
Hannigan, J.; Palm, M.; Conway, S. et al

Conference (2015, October 05)

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See detailPhysicochimie de la pollution atmosphérique
Mahieu, Emmanuel ULg

Conference (2015, September 25)

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See detailAcetylene (C2H2) and hydrogen cyanide (HCN) from IASI satellite observations: global distributions, validation, and comparison with model
Duflot, V.; Wespes, C.; Clarisse, L. et al

in Atmospheric Chemistry and Physics (2015), 15

We present global distributions of C2H2 and hydrogen cyanide (HCN) total columns derived from the Infrared Atmospheric Sounding Interferometer (IASI) for the years 2008–2010. These distributions are ... [more ▼]

We present global distributions of C2H2 and hydrogen cyanide (HCN) total columns derived from the Infrared Atmospheric Sounding Interferometer (IASI) for the years 2008–2010. These distributions are obtained with a fast method allowing to retrieve C2H2 abundance globally with a 5% precision and HCN abundance in the tropical (subtropical) belt with a 10% (25 %) precision. IASI data are compared for validation purposes with ground-based Fourier transform infrared (FTIR) spectrometer measurements at four selected stations. We show that there is an overall agreement between the ground-based and space measurements with correlation coefficients for daily mean measurements ranging from 0.28 to 0.81, depending on the site. Global C2H2 and subtropical HCN abundances retrieved from IASI spectra show the expected seasonality linked to variations in the anthropogenic emissions and seasonal biomass burning activity, as well as exceptional events, and are in good agreement with previous spaceborne studies. Total columns simulated by the Model for Ozone and Related Chemical Tracers, version 4 (MOZART-4) are compared to the ground-based FTIR measurements at the four selected stations. The model is able to capture the seasonality in the two species in most of the cases, with correlation coefficients for daily mean measurements ranging from 0.50 to 0.86, depending on the site. IASI measurements are also compared to the distributions from MOZART-4. Seasonal cycles observed from satellite data are reasonably well reproduced by the model with correlation coefficients ranging from -0.31 to 0.93 for C2H2 daily means, and from 0.09 to 0.86 for HCN daily means, depending on the considered region. However, the anthropogenic (biomass burning) emissions used in the model seem to be overestimated (underestimated), and a negative global mean bias of 1% (16 %) of the model relative to the satellite observations was found for C2H2 (HCN). [less ▲]

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See detailStratospheric HCl increasing again, caused by dynamic variability, driven by increased tropopsheric wave activity
Notholt, J; Mahieu, Emmanuel ULg; Pfloeger, F et al

Conference (2015, September 22)

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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 and Physics (2015), 15(17), 9965--9982

Trends in the vertical distribution of ozone are reported and compared for a number of new and recently revised data sets. 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 data sets. The amount of ozone-depleting compounds in the stratosphere (as measured by equivalent effective stratospheric chlorine – EESC) was maximised in the second half of the 1990s. We examine the periods before and after the peak to see if any change in trend is discernible in the ozone record that might be attributable to a change in the EESC trend, though no attribution is attempted. 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 main satellite and groundbased records 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 data sets. The averaged upward trends are significant if the trends derived from various data sets are assumed to be independent (as in Pawson et al., 2014) but are generally not significant if the trends are not independent. This occurs because many of the underlying measurement records are used in more than one merged data set. 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 detailAtmospheric circulation changes identified thanks to ground-based FTIR monitoring of hydrogen chloride (HCl)
Mahieu, Emmanuel ULg; Chipperfield, Martyn. P.; Notholt, Justus et al

Article for general public (2015)

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See detailSurveillance à long terme de l'atmosphère terrestre depuis la station du Jungfraujoch
Mahieu, Emmanuel ULg

Conference (2015, July 02)

Nous présentons une vue d'ensemble des activités menées par les chercheurs de l'Université de Liège à la station scientifique internationale du Jungfraujoch, depuis les observations infrarouges pionnières ... [more ▼]

Nous présentons une vue d'ensemble des activités menées par les chercheurs de l'Université de Liège à la station scientifique internationale du Jungfraujoch, depuis les observations infrarouges pionnières effectuées à ce site par le Pr Migeotte en 1950-1951. L'accent est mis sur les données géophysiques et les séries temporelles déduites pour les constituants de l'atmosphère influençant le climat. [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 detailRemote sensing of the atmospheric composition in the infrared spectral region within the Network for the Detection of Atmospheric Composition Change (NDACC) and the Total Carbon Column Observing Network (TCCON)
Notholt, J; Blumenstock, T; Deutscher, N et al

Conference (2015, May 12)

Remote sensing has been established as a powerful tool in atmospheric research. Throughout the last decades satellite and ground-based remote sensing instruments and methods have been developed to sample ... [more ▼]

Remote sensing has been established as a powerful tool in atmospheric research. Throughout the last decades satellite and ground-based remote sensing instruments and methods have been developed to sample the atmosphere from the microwave to the UV/Vis. The international ground based networks NDACC-IR and TCCON are based on solar absorption spectrometry in the infrared. Both networks consist of more than 30 observations sites around the globe, from the high Arctic through mid-latitudes and the tropics to the southern hemisphere and Antarctica. NDACC concentrates on stratospheric observations in relation to ozone chemistry, in many instances, information on the vertical distribution of the target species is determined. Measured trace gases include O3, HCl, HF, HNO3, ClONO2 and many others. In addition, the tropospheric composition is studied by measuring anthropogenic and biogenic species including HCN, OCS, H2O, CO, CH2O, C2H6, and C2H2. The aim of TCCON is to acquire accurate and precise column-averaged abundances of CO2, CH4, N2O, i.e. atmospheric trace gases which have a very small natural variability. TCCON measurements are linked to WMO calibration scales by comparisons with co-incident in situ profiles measured from aircraft or balloon. Results from both networks have been used in many studies in relation to stratospheric ozone chemistry, air-pollution, and with regard to the carbon-cycle. Long-term series are necessary for trend analysis, gaining insight into annual and longer term variability and placing into context shorter term process studies. Due to the similar observation geometry, the ground-based observations are optimally suitable for satellite and model validation and form an essential part of many satellite projects. They also play an important role in the validation of the Copernicus Atmospheric Monitoring Service. In our contribution we will give an overview on the current status of both networks, ongoing efforts to improve network coverage, precision and accuracy, and several examples of scientific highlights. [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 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 (2015), 8(4), 1799-1818

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 data set from the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY). The data set is extended with 2 additional years, now covering 2003–2007, and is validated against co-located ground-based total column δD 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 among the available data is not yet ideal, we determined a mean negative bias in SCIAMACHY δD 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 (∼ −60 to −80‰) at the highest latitudes and smallest (∼ −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 δD 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 δD 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 vapour and shows the added information that HDO/H2O measurements provide when 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 (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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