References of "Mahieu, Emmanuel"
     in
Bookmark and Share    
Full Text
Peer Reviewed
See detailGround-based FTIR retrievals of SF6 at Réunion Island
Zhou, M.; Langerock, B.; Vigouroux, C. et al

in Atmospheric Measurement Techniques. Papers in Open Discussion (2017), 2017

SF6 total columns are successfully retrieved from FTIR measurements (Saint Denis and Maïdo) at Réunion Island (21 S, 55 E) between 2004-2016 using the SFIT4 algorithm: the retrieval strategy and the error ... [more ▼]

SF6 total columns are successfully retrieved from FTIR measurements (Saint Denis and Maïdo) at Réunion Island (21 S, 55 E) between 2004-2016 using the SFIT4 algorithm: the retrieval strategy and the error budget are presented. The FTIR SF6 retrieval has independent information in only one individual layer, covering the whole troposphere and the lower stratosphere. The trend of SF6 is analysed based on the FTIR retrieved dry air column-averaged mole fractions (XSF6 ) at Réunion Island, the in-situ measurements at America Samoa (SMO) and the collocated satellite measurements (MIPAS and ACE-FTS) in the southern tropics. The SF6 annual growth rate from FTIR retrievals is 0.265±0.013 pptv/year for 2004–2016, which is slightly weaker than that from the SMO in-situ measurements (0.285±0.002 pptv/year) for the same time period. The SF6 trend in the troposphere from MIPAS and ACE-FTS observations is also close to the ones from the FTIR retrievals and the SMO in-situ measurements. [less ▲]

Detailed reference viewed: 37 (1 ULiège)
Full Text
Peer Reviewed
See detailSurveillance de l'atmosphère terrestre depuis la station du Jungfraujoch : une épopée liégeoise entamée voici plus de 65 ans !
Mahieu, Emmanuel ULiege; Bader, Whitney ULiege; Bovy, Benoît ULiege et al

in Bulletin de la Société Géographique de Liège (2017), 68

It’s in the early 1950s that researchers from the University of Liège started to investigate the Earth’s atmosphere from the Jungfraujoch scientific station, in the Swiss Alps, at a time when concerns ... [more ▼]

It’s in the early 1950s that researchers from the University of Liège started to investigate the Earth’s atmosphere from the Jungfraujoch scientific station, in the Swiss Alps, at a time when concerns related to atmospheric composition changes were nonexistent. Since then, an infrared observational data base unique worldwide has been carefully collected. The exploitation of these observations has allowed constituting multi-decadal time series crucial for the characterization of the changes that affected our atmosphere and for the identification of their causes. In this paper, we first remind about the successive steps which led to establishing the observational program of the Liège team at the Jungfraujoch and we evoke important findings which justified its continuation. Then we present some recent results relevant to the Montreal and Kyoto Protocols, or related to the monitoring of air quality. [less ▲]

Detailed reference viewed: 25 (3 ULiège)
Full Text
Peer Reviewed
See detailAn update on ozone profile trends for the period 2000 to 2016
Steinbrecht, Wolfgang; Froidevaux, Lucien; Fuller, Ryan et al

in Atmospheric Chemistry and Physics (2017), 17(17), 10675-10690

Ozone profile trends over the period 2000 to 2016 from several merged satellite ozone data sets and from ground-based data by four techniques at stations of the Network for the Detection of Atmospheric ... [more ▼]

Ozone profile trends over the period 2000 to 2016 from several merged satellite ozone data sets and from ground-based data by four techniques at stations of the Network for the Detection of Atmospheric Composition Change indicate significant ozone increases in the upper stratosphere, between 35 and 48 km altitude (5 and 1 hPa). Near 2 hPa (42 km), ozone has been increasing by about 1.5 % per decade in the tropics (20°S to 20°N), and by 2 to 2.5 % per decade in the 35° to 60° latitude bands of both hemispheres. At levels below 35 km (5 hPa), 2000 to 2016 ozone trends are smaller and not statistically significant. The observed trend profiles are consistent with expectations from chemistry climate model simulations. Using three to four more years of observations and updated data sets, this study confirms positive trends of upper stratospheric ozone already reported, e.g., in the WMO/UNEP Ozone Assessment 2014, or by Harris et al. (2015). The additional years, and the fact that nearly all individual data sets indicate these increases, give enhanced confidence. Nevertheless, a thorough analysis of possible drifts and differences between various data sources is still required, as is a detailed attribution of the observed increases to declining ozone depleting substances and to stratospheric cooling. Ongoing quality observations from multiple independent platforms are key for verifying that recovery of the ozone layer continues as expected. [less ▲]

Detailed reference viewed: 24 (1 ULiège)
Full Text
See detailAtmospheric free acidity from cloud processing
Franco, Bruno ULiege; Taraborrelli, Domenico; Gromov, Sergey et al

Conference (2017, June 27)

Detailed reference viewed: 40 (5 ULiège)
Full Text
Peer Reviewed
See detailValidation of MOPITT carbon monoxide using ground-based Fourier transform infrared spectrometer data from NDACC
Buchholz, R. R.; Deeter, M. N.; Worden, H. M. et al

in Atmospheric Measurement Techniques (2017), 10(5), 1927--1956

The Measurements of Pollution in the Troposphere (MOPITT) satellite instrument provides the longest continuous dataset of carbon monoxide (CO) from space. We perform the first validation of MOPITT version ... [more ▼]

The Measurements of Pollution in the Troposphere (MOPITT) satellite instrument provides the longest continuous dataset of carbon monoxide (CO) from space. We perform the first validation of MOPITT version 6 retrievals using total column CO measurements from ground-based remote-sensing Fourier transform infrared spectrometers (FTSs). Validation uses data recorded at 14 stations, that span a wide range of latitudes (80°N to 78°S), in the Network for the Detection of Atmospheric Composition Change (NDACC). MOPITT measurements are spatially co-located with each station, and different vertical sensitivities between instruments are accounted for by using MOPITT averaging kernels (AKs). All three MOPITT retrieval types are analyzed: thermal infrared (TIR-only), joint thermal and near infrared (TIR–NIR), and near infrared (NIR-only). Generally, MOPITT measurements overestimate CO relative to FTS measurements, but the bias is typically less than 10%. Mean bias is 2.4% for TIR-only, 5.1% for TIR–NIR, and 6.5% for NIR-only. The TIR–NIR and NIR-only products consistently produce a larger bias and lower correlation than the TIR-only. Validation performance of MOPITT for TIR-only and TIR–NIR retrievals over land or water scenes is equivalent. The four MOPITT detector element pixels are validated separately to account for their different uncertainty characteristics. Pixel 1 produces the highest standard deviation and lowest correlation for all three MOPITT products. However, for TIR-only and TIR–NIR, the error-weighted average that includes all four pixels often provides the best correlation, indicating compensating pixel biases and well-captured error characteristics. We find that MOPITT bias does not depend on latitude but rather is influenced by the proximity to rapidly changing atmospheric CO. MOPITT bias drift has been bound geographically to within ±0.5%/yr or lower at almost all locations. [less ▲]

Detailed reference viewed: 41 (3 ULiège)
Full Text
See detailObservation and simulation of ethane at 22 FTIR sites
Mahieu, Emmanuel ULiege; Franco, Bruno ULiege; Pozzer, Andrea et al

Conference (2017, May 30)

Detailed reference viewed: 68 (6 ULiège)
Full Text
See detailImpact of circulation changes on the long-term trend of stratospheric hydrogen fluoride at five NDACC stations
Prignon, Maxime ULiege; Bernath, P.F.; Blumenstock, T. et al

Poster (2017, May 29)

Hydrogen fluoride is mainly produced by the photolysis of anthropogenic source gases such as the chlorofluorocarbons (CFC), the hydrochlorofluorocarbons (HCFC) and the hydrofluorocarbons (HFC). These ... [more ▼]

Hydrogen fluoride is mainly produced by the photolysis of anthropogenic source gases such as the chlorofluorocarbons (CFC), the hydrochlorofluorocarbons (HCFC) and the hydrofluorocarbons (HFC). These families of species are known for contributing to ozone depletion and/or to the greenhouse effect. It is thus essential to regulate and monitor their emissions. Despite the fact that the Montreal protocol (1987) has succeeded to reduce and then suppress the CFC emissions, HF is still increasing in the stratosphere because of ongoing emissions of the HCFC and HFC substitution products. In the framework of the recent studies demonstrating the influence of stratospheric circulation changes on the trend of long-lived tracers (e.g. hydrogen chlorine), we decided to investigate the impact of these circulation changes on HF. To achieve this objective, the rates of changes over time of HF total/partial columns at various latitudes of the globe will be determined and critically discussed. Fourier Transform Infrared data produced at five NDACC sites (Kiruna – 68°N, Jungfraujoch – 46°N, Izana – 28°N, Lauder 45°S and Arrival-heights – 78°S) and satellite data (HALOE and ACE) will be used for this study. This preliminary selection of ground-based stations allows to cover both hemispheres and our period of investigation (last two decades). Finally, in order to support our data interpretation, two SLIMCAT simulations (standard and fixed dynamics) will also be included. [less ▲]

Detailed reference viewed: 32 (6 ULiège)
Full Text
Peer Reviewed
See detailRevisiting global fossil fuel and biofuel emissions of ethane
Tzompa-Sosa, Z. A.; Mahieu, Emmanuel ULiege; Franco, Bruno ULiege et al

in Journal of Geophysical Research. Atmospheres (2017), 122(4), 2493--2512

Recent measurements over the Northern Hemisphere indicate that the long-term decline in the atmospheric burden of ethane (C2H6) has ended and the abundance increased dramatically between 2010 and 2014 ... [more ▼]

Recent measurements over the Northern Hemisphere indicate that the long-term decline in the atmospheric burden of ethane (C2H6) has ended and the abundance increased dramatically between 2010 and 2014. The rise in C2H6 atmospheric abundances has been attributed to oil and natural gas extraction in North America. Existing global C2H6 emission inventories are based on outdated activity maps that do not account for current oil and natural gas exploitation regions. We present an updated global C2H6 emission inventory based on 2010 satellite-derived CH4 fluxes with adjusted C2H6 emissions over the U.S. from the National Emission Inventory (NEI 2011). We contrast our global 2010 C2H6 emission inventory with one developed for 2001. The C2H6 difference between global anthropogenic emissions is subtle (7.9 versus 7.2 Tg yr−1), but the spatial distribution of the emissions is distinct. In the 2010 C2H6 inventory, fossil fuel sources in the Northern Hemisphere represent half of global C2H6 emissions and 95% of global fossil fuel emissions. Over the U.S., unadjusted NEI 2011 C2H6 emissions produce mixing ratios that are 14–50% of those observed by aircraft observations (2008–2014). When the NEI 2011 C2H6 emission totals are scaled by a factor of 1.4, the Goddard Earth Observing System Chem model largely reproduces a regional suite of observations, with the exception of the central U.S., where it continues to underpredict observed mixing ratios in the lower troposphere. We estimate monthly mean contributions of fossil fuel C2H6 emissions to ozone and peroxyacetyl nitrate surface mixing ratios over North America of ~1% and ~8%, respectively. [less ▲]

Detailed reference viewed: 16 (2 ULiège)
Full Text
Peer Reviewed
See detailThe recent increase of atmospheric methane from 10 years of ground-based NDACC FTIR observations since 2005
Bader, Whitney ULiege; Bovy, Benoît ULiege; Conway, Stephanie et al

in Atmospheric Chemistry and Physics (2017)

Changes of atmospheric methane total columns (CH4/ since 2005 have been evaluated using Fourier transform infrared (FTIR) solar observations carried out at 10 ground-based sites, affiliated to the Network ... [more ▼]

Changes of atmospheric methane total columns (CH4/ since 2005 have been evaluated using Fourier transform infrared (FTIR) solar observations carried out at 10 ground-based sites, affiliated to the Network for Detection of Atmospheric Composition Change (NDACC). From this, we find an increase of atmospheric methane total columns of 0.31±0.03 %/year (2-sigma level of uncertainty) for the 2005–2014 period. Comparisons with in situ methane measurements at both local and global scales show good 10 agreement. We used the GEOS-Chem chemical transport model tagged simulation, which accounts for the contribution of each emission source and one sink in the total methane, simulated over 2005–2012. After regridding according to NDACC vertical layering using a conservative 15 regridding scheme and smoothing by convolving with respective FTIR seasonal averaging kernels, the GEOS-Chem simulation shows an increase of atmospheric methane total columns of 0.35±0.03 %/year between 2005 and 2012, which is in agreement with NDACC measurements over the same time period (0.30±0.04 %/year, averaged over 10 stations). Analysis of the GEOS-Chem-tagged simulation allows us to quantify the contribution of each tracer to the global methane change since 2005. We find that natural sources such as wetlands and biomass burning contribute to the interannual variability of methane. However, anthropogenic emissions, such as coal mining, and gas and oil transport and exploration, which are mainly emitted in the Northern Hemisphere and act as secondary contributors to the global budget of methane, have played a major role in the increase of atmospheric methane observed since 2005. Based on the GEOS-Chem-tagged simulation, we discuss possible cause(s) for the increase of methane since 2005, which is still unexplained. [less ▲]

Detailed reference viewed: 73 (10 ULiège)
Full Text
Peer Reviewed
See detailTropospheric water vapour isotopologue data (H216O, H218O and HD16O) as obtained from NDACC/FTIR solar absorption spectra
Barthlott, Sabine; Schneider, Matthias; Hase, Frank et al

in Earth System Science Data (2017), 9

We report on the ground-based FTIR (Fourier Transform InfraRed) tropospheric water vapour isotopologue remote sensing data that have been recently made available via the database of NDACC (Network for the ... [more ▼]

We report on the ground-based FTIR (Fourier Transform InfraRed) tropospheric water vapour isotopologue remote sensing data that have been recently made available via the database of NDACC (Network for the Detection of Atmospheric Composition Change; ftp://ftp.cpc.ncep.noaa.gov/ndacc/MUSICA/) and via doi:10.5281/zenodo.48902. Currently, data are available for 12 globally distributed stations. They have been centrally retrieved and quality filtered in the framework of the MUSICA project (MUlti-platform remote Sensing of Isotopologues for investigating the Cycle of Atmospheric water). We explain particularities of retrieving the water vapour isotopologue state (vertical distribution of H162O, H182O and HD16O) and reveal the need for a new meta-data template for archiving FTIR isotopologue data. We describe the format of different data components and give recommendations for correct data usage. Data are provided as two data types. The first type is best-suited for tropospheric water vapour distribution studies disregarding different isotopologues (comparison with radiosonde data, analyses of water vapour variability and trends, etc.). The second type is needed for analysing moisture pathways by means of {H2O,delta-D}-pair distributions. [less ▲]

Detailed reference viewed: 88 (7 ULiège)
Full Text
Peer Reviewed
See detailOptimized approach to retrieve information on atmospheric carbonyl sulfide (OCS) above the Jungfraujoch station and change in its abundance since 1995
Lejeune, Bernard ULiege; Mahieu, Emmanuel ULiege; Vollmer, M. K. et al

in Journal of Quantitative Spectroscopy & Radiative Transfer (2017), 186

In this paper, we present an optimized retrieval strategy for carbonyl sulfide (OCS), using Fourier transform infrared (FTIR) solar observations made at the high-altitude Jungfraujoch station in the Swiss ... [more ▼]

In this paper, we present an optimized retrieval strategy for carbonyl sulfide (OCS), using Fourier transform infrared (FTIR) solar observations made at the high-altitude Jungfraujoch station in the Swiss Alps. More than 200 lines of the nu3 fundamental band of OCS have been systematically evaluated and we selected 4 microwindows on the basis of objective criteria minimizing the effect of interferences, mainly by solar features, carbon dioxide and water vapor absorption lines, while maximizing the information content. Implementation of this new retrieval strategy provided an extended time series of the OCS abundance spanning the 1995-2015 time period, for the study of the long-term trend and seasonal variation of OCS in the free troposphere and stratosphere. Three distinct periods characterize the evolution of the tropospheric partial columns: a first decreasing period (1995-2002), an intermediate increasing period (2002-2008), and the more recent period (2008-2015) which shows no significant trend. Our FTIR tropospheric and stratospheric time series are compared with new in situ gas chromatography mass spectrometry (GCMS) measurements performed by Empa (Laboratory for Air Pollution/Environmental Technology) at the Jungfraujoch since 2008, and with space-borne solar occultation observations by the ACE-FTS instrument on-board the SCISAT satellite, respectively, and they show good agreement. The OCS signal recorded above Jungfraujoch appears to be closely related to anthropogenic sulfur emissions. [less ▲]

Detailed reference viewed: 103 (27 ULiège)
Full Text
Peer Reviewed
See detailModel Sensitivity Studies of the Decrease in Atmospheric Carbon Tetrachloride
Chipperfield, M. P.; Liang, Q.; Rigby, M. et al

in Atmospheric Chemistry and Physics (2016), 16

Carbon tetrachloride is an ozone-depleting substance, which is controlled by the Montreal Protocol and for which the atmospheric abundance is decreasing. However, the current observed rate of this ... [more ▼]

Carbon tetrachloride is an ozone-depleting substance, which is controlled by the Montreal Protocol and for which the atmospheric abundance is decreasing. However, the current observed rate of this decrease is known to be slower than expected based on reported CCl4 emissions and its estimated overall atmospheric lifetime. Here we use a three-dimensional (3-D) chemical transport model to investigate the impact on its predicted decay of uncertainties in the rates at which CCl4 is removed from the atmosphere by photolysis, by ocean uptake and by degradation in soils. The largest sink is atmospheric photolysis (76% of total) but a reported 10% uncertainty in its combined photolysis cross-section and quantum yield has only a modest impact on the modelled rate of CCl4 decay. This is partly due to the limiting effect of the rate of transport of CCl4 from the main tropospheric reservoir to the stratosphere where photolytic loss occurs. The model suggests large interannual variability in the magnitude of this stratospheric photolysis sink caused by variations in transport. The impact of uncertainty in the minor soil sink (9% of total) is also relatively small. In contrast, the model shows that uncertainty in ocean loss (15% of total) has the largest impact on modelled CCl4 decay due to its sizeable contribution to CCl4 loss and large uncertainty range (157 to 313 years). With an assumed CCl4 emission rate of 39 Gg/yr, the reference simulation with best estimate of loss processes still underestimates the observed CCl4 (overestimates the decay) over the past two decades but to a smaller extent than previous studies. Changes to the rate of CCl4 loss processes, in line with known uncertainties, could bring the model into agreement with in situ surface and remote-sensing measurements, as could an increase in emissions to around 45 Gg/yr. Further progress in constraining the CCl4 budget is partly limited by systematic biases between observational datasets. For example, surface observations from the NOAA network are larger than from the AGAGE network but have shown a steeper decreasing trend over the past two decades. These differences imply a difference in emissions which is significant relative to uncertainties in the magnitudes of the CCl4 sinks. [less ▲]

Detailed reference viewed: 65 (1 ULiège)
Full Text
Peer Reviewed
See detailFirst characterization and validation of FORLI-HNO3 vertical profiles retrieved from IASI/Metop
Ronsmans, G.; Langerock, B.; Wespes, C. et al

in Atmospheric Measurement Techniques (2016), 16

Knowing the spatial and seasonal distributions of nitric acid (HNO3) around the globe is of great interest to apprehend the processes regulating stratospheric ozone, especially in the polar regions ... [more ▼]

Knowing the spatial and seasonal distributions of nitric acid (HNO3) around the globe is of great interest to apprehend the processes regulating stratospheric ozone, especially in the polar regions. Thanks to its unprecedented spatial and temporal sampling, the nadir-viewing Infrared Atmospheric Sounding Interferometer (IASI) allows sounding the atmosphere twice a day globally, with good spectral resolution and low noise. With the Fast Optimal Retrievals on Layers for IASI (FORLI) algorithm, we are retrieving, in near-real time, columns as well as vertical profiles of several atmospheric species, amongst which is HNO3. We present in this paper the first characterization of the FORLI-HNO3 profile products, in terms of vertical sensitivity and error budgets. We show that the sensitivity of IASI to HNO3 is highest in the lower stratosphere (10–20km), where the largest amounts of HNO3 are found, but that the vertical sensitivity of IASI only allows one level of information on the profile (DOFS 1). The sensitivity near the surface is negligible in most cases, and for this reason, a partial column (5–35km) is used for the analyses. Both vertical profiles and partial columns are compared to FTIR ground-based measurements from the Network for the Detection of Atmospheric Composition Change (NDACC) to characterize the accuracy and precision of the FORLI-HNO3 product. The profile validation is conducted through the smoothing of the raw FTIR profiles by the IASI averaging kernels and gives good results, with a slight overestimation of IASI measurements in the Upper Troposphere-Lower Stratosphere (UTLS) at the 6 chosen stations (Thule, Kiruna, Jungfraujoch, Izaña, Lauder and Arrival Heights). The validation of the partial columns (5–35km) is also conclusive with a mean correlation of 0.93 between IASI and the FTIR measurements. An initial survey of the HNO3 spatial and seasonal variabilities obtained from IASI measurements for a one year (2011) data set shows that the expected latitudinal gradient of concentrations from low to high latitudes and the large seasonal variability in polar regions (cycle amplitude around 30% of the seasonal signal, peak-to-peak) are well represented with IASI data. [less ▲]

Detailed reference viewed: 39 (9 ULiège)
Full Text
Peer Reviewed
See detailSeasonal variability of surface and column carbon monoxide over megacity Paris, high-altitude Jungfraujoch and Southern Hemispheric Wollongong stations
Té, Y; Jeseck, P; Franco, Bruno ULiege et al

in Atmospheric Chemistry and Physics (2016), 16

This paper studies the seasonal variation of surface and column CO at three different sites (Paris, Jungfraujoch and Wollongong), with an emphasis on establishing a link between the CO vertical ... [more ▼]

This paper studies the seasonal variation of surface and column CO at three different sites (Paris, Jungfraujoch and Wollongong), with an emphasis on establishing a link between the CO vertical distribution and the nature of CO emission sources. We find the first evidence of a time lag between surface and free tropospheric CO seasonal variations in the Northern Hemisphere. The CO seasonal variability obtained from the total columns and free tropospheric partial columns shows a maximum around March–April and a minimum around September–October in the Northern Hemisphere (Paris and Jungfraujoch). In the Southern Hemisphere (Wollongong) this seasonal variability is shifted by about 6 months. Satellite observations by the IASI–MetOp (Infrared Atmospheric Sounding Interferometer) and MOPITT (Measurements Of Pollution In The Troposphere) instruments confirm this seasonality. Ground-based FTIR (Fourier transform infrared) measurements provide useful complementary information due to good sensitivity in the boundary layer. In situ surface measurements of CO volume mixing ratios at the Paris and Jungfraujoch sites reveal a time lag of the near-surface seasonal variability of about 2 months with respect to the total column variability at the same sites. The chemical transport model GEOS-Chem (Goddard Earth Observing System chemical transport model) is employed to interpret our observations. GEOS-Chem sensitivity runs identify the emission sources influencing the seasonal variation of CO. At both Paris and Jungfraujoch, the surface seasonality is mainly driven by anthropogenic emissions, while the total column seasonality is also controlled by air masses transported from distant sources. At Wollongong, where the CO seasonality is mainly affected by biomass burning, no time shift is observed between surface measurements and total column data. [less ▲]

Detailed reference viewed: 103 (9 ULiège)
Full Text
Peer Reviewed
See detailIntercomparison of in-situ NDIR and column FTIR measurements of CO2 at Jungfraujoch
Schibig, M. F.; Mahieu, Emmanuel ULiege; Henne, S. et al

in Atmospheric Chemistry and Physics (2016), 16(15), 9935--9949

We compare two CO2 time series measured at the High Alpine Research Station Jungfraujoch, Switzerland (3580 m a.s.l.), in the period from 2005 to 2013 with an in situ surface measurement system using a ... [more ▼]

We compare two CO2 time series measured at the High Alpine Research Station Jungfraujoch, Switzerland (3580 m a.s.l.), in the period from 2005 to 2013 with an in situ surface measurement system using a nondispersive infrared analyzer (NDIR) and a ground-based remote sensing system using solar absorption Fourier transform infrared (FTIR) spectrometry. Although the two data sets show an absolute shift of about 13 ppm, the slopes of the annual CO2 increase are in good agreement within their uncertainties. They are 2.04±0.07 and 1.97±0.05 ppm yr-1 for the FTIR and the NDIR systems, respectively. The seasonality of the FTIR and the NDIR systems is 4.46±1.11 and 10.10±0.73 ppm, respectively. The difference is caused by a dampening of the CO2 signal with increasing altitude due to mixing processes. Whereas the minima of both data series occur in the middle of August, the maxima of the two data sets differ by about 10 weeks; the maximum of the FTIR measurements is in the middle of January, and the maximum of the NDIR measurements is found at the end of March. Sensitivity analyses revealed that the air masses measured by the NDIR system at the surface of Jungfraujoch are mainly influenced by central Europe, whereas the air masses measured by the FTIR system in the column above Jungfraujoch are influenced by regions as far west as the Caribbean and the USA. The correlation between the hourly averaged CO2 values of the NDIR system and the individual FTIR CO2 measurements is 0.820, which is very encouraging given the largely different sampling volumes. Further correlation analyses showed, that the correlation is mainly driven by the annual CO2 increase and to a lesser degree by the seasonality. Both systems are suitable to monitor the long-term CO2 increase, because this signal is represented in the whole atmosphere due to mixing. [less ▲]

Detailed reference viewed: 77 (18 ULiège)
Full Text
Peer Reviewed
See detailHCOOH distributions from IASI for 2008-2014: comparison with ground-based FTIR measurements and a global chemistry-transport model
Pommier, M.; Clerbaux, C.; Coheur, P.-F. et al

in Atmospheric Chemistry and Physics (2016), 16

Formic acid (HCOOH) is one of the most abundant volatile organic compounds in the atmosphere. It is a major contributor to rain acidity in remote areas. There are, however, large uncertainties on the ... [more ▼]

Formic acid (HCOOH) is one of the most abundant volatile organic compounds in the atmosphere. It is a major contributor to rain acidity in remote areas. There are, however, large uncertainties on the sources and sinks of HCOOH and therefore HCOOH is misrepresented by global chemistry-transport models. This work presents global distributions from 2008 to 2014 as derived from the measurements of the Infrared Atmospheric Sounding Interferometer (IASI), based on conversion factors between brightness temperature differences and representative retrieved total columns over seven regions: Northern Africa, southern Africa, Amazonia, Atlantic, Australia, Pacific, and Russia. The dependence of the measured HCOOH signal on the thermal contrast is taken into account in the conversion method. This conversion presents errors lower than 20 % for total columns ranging between 0.5 and 1 × 1016 molec/cm2 but reaches higher values, up to 78 %, for columns that are lower than 0.3 × 1016 molec/cm2. Signatures from biomass burning events are highlighted, such as in the Southern Hemisphere and in Russia, as well as biogenic emission sources, e.g., over the eastern USA. A comparison between 2008 and 2014 with ground-based Fourier transform infrared spectroscopy (FTIR) measurements obtained at four locations (Maido and Saint-Denis at La Réunion, Jungfraujoch, and Wollongong) is shown. Although IASI columns are found to correlate well with FTIR data, a large bias (> 100 %) is found over the two sites at La Réunion. A better agreement is found at Wollongong with a negligible bias. The comparison also highlights the difficulty of retrieving total columns from IASI measurements over mountainous regions such as Jungfraujoch. A comparison of the retrieved columns with the global chemistry-transport model IMAGESv2 is also presented, showing good representation of the seasonal and interannual cycles over America, Australia, Asia, and Siberia. A global model underestimation of the distribution and a misrepresentation of the seasonal cycle over India are also found. A small positive trend in the IASI columns is observed over Australia, Amazonia, and India over the 2008–2014 period (from 0.7 to 1.5 %/year), while a decrease of ∼ 0.8 %/year is measured over Siberia. [less ▲]

Detailed reference viewed: 53 (5 ULiège)
Full Text
Peer Reviewed
See detailSPARC Report on the Mystery of Carbon Tetrachloride
Ahmadzai, H; Bock, R P; Burkholder, J B et al

in Liang, Qing; Newman, Paul A; Reimann, Stefan (Eds.) SPARC Report on the Mystery of Carbon Tetrachloride (2016)

The Montreal Protocol (MP) controls the production and consumption of carbon tetrachloride (CCl4 or CTC) and other ozone-depleting substances (ODSs) for emissive uses. CCl4 is a major ODS, accounting for ... [more ▼]

The Montreal Protocol (MP) controls the production and consumption of carbon tetrachloride (CCl4 or CTC) and other ozone-depleting substances (ODSs) for emissive uses. CCl4 is a major ODS, accounting for about 12% of the globally averaged inorganic chlorine and bromine in the stratosphere, compared to 14% for CFC-12 in 2012. In spite of the MP controls, there are large ongoing emissions of CCl4 into the atmosphere. Estimates of emissions from various techniques ought to yield similar numbers. However, the recent WMO/UNEP Scientific Assessment of Ozone Depletion [WMO, 2014] estimated a 2007-2012 CCl4 bottom-up emission of 1-4 Gg/year (1-4 kilotonnes/year), based on country-by-country reports to UNEP, and a global top-down emissions estimate of 57 Gg/ year, based on atmospheric measurements. This 54 Gg/year difference has not been explained. In order to assess the current knowledge on global CCl4 sources and sinks, stakeholders from industrial, governmental, and the scientific communities came together at the “Solving the Mystery of Carbon Tetrachloride” workshop, which was held from 4-6 October 2015 at Empa in Dübendorf, Switzerland. During this workshop, several new findings were brought forward by the participants on CCl4 emissions and related science. • Anthropogenic production and consumption for feedstock and process agent uses (e.g., as approved solvents) are reported to UNEP under the MP. Based on these numbers, global bottom-up emissions of 3 (0-8) Gg/year are estimated for 2007-2013 in this report. This number is also reasonably consistent with this report’s new industry-based bottom-up estimate for fugitive emissions of 2 Gg/year. • By-product emissions from chloromethanes and perchloroethylene plants are newly proposed in this report as significant CCl4 sources, with global emissions estimated from these plants to be 13 Gg/year in 2014. • This report updates the anthropogenic CCl4 emissions estimation as a maximum of ~25 Gg/year. This number is derived by combining the above fugitive and by-product emissions (2 Gg/year and 13 Gg/year, respectively) with 10 Gg/year from legacy emissions plus potential unreported inadvertent emissions from other sources. • Ongoing atmospheric CCl4 measurements within global networks have been exploited for assessing regional emissions. In addition to existing emissions estimates from China and Australia, the workshop prompted research on emissions in the U.S. and Europe. The sum of these four regional emissions is estimated as 21±7.5a Gg/year, but this is not a complete global accounting. These regional top-down emissions estimates also show that most of the CCl4 emissions originate from chemical industrial regions, and are not linked to major population centres. • The total CCl4 lifetime is critical for calculating top-down global emissions. CCl4 is destroyed in the stratosphere, oceans, and soils, complicating the total lifetime estimate. The atmospheric lifetime with respect to stratospheric loss was recently revised to 44 (36-58) years, and remains unchanged in this report. New findings from additional measurement campaigns and reanalysis of physical parameters lead to changes in the ocean lifetime from 94 years to 210 (157-313) years, and in the soil lifetime from 195 years to 375 (288-536) years. • These revised lifetimes lead to an increase of the total lifetime from 26 years in WMO [2014] to 33 (28-41) years. Consequently, CCl4 is lost at a slower rate from the atmosphere. With this new total lifetime, the global top-down emissions calculation decreases from 57 (40-74) Gg/year in WMO [2014] to 40 (25-55) Gg/year. This estimate is relatively consistent with the independent gradient top-down emissions of 30 (25-35) Gg/year, based upon differences between atmospheric measurements of CCl4 in the Northern and Southern Hemispheres. In addition, this new total lifetime implies an upper limit of 3-4 Gg/year of natural emissions, based upon newly reported observations of old air in firn snow. These new CCl4 emissions estimates from the workshop make considerable progress toward closing the emissions discrepancy. The new industrial bottom-up emissions estimate (15 Gg/year total) includes emissions from chloromethanes plants (13 Gg/year) and feedstock fugitive emissions (2 Gg/year). When combined with legacy emissions and unreported inadvertent emissions, this could be up to 25 Gg/year. Top-down emissions estimates are: global 40 (25-55) Gg/year, gradient 30 (25-35) Gg/year, and regional 21 (14-28) Gg/year. While the new bottom-up value is still less than the aggregated top-down values, these estimates reconcile the CCl4 budget discrepancy when considered at the edges of their uncertainties. [less ▲]

Detailed reference viewed: 99 (6 ULiège)
Full Text
Peer Reviewed
See detailReversal of global atmospheric ethane and propane trends largely due to US oil and natural gas production
Helmig, Detlev; Rossabi, Samuel; Hueber, Jacques et al

in Nature Geoscience (2016)

Non-methane hydrocarbons such as ethane are important precursors to tropospheric ozone and aerosols. Using data from a global surface network and atmospheric column observations we show that the steady ... [more ▼]

Non-methane hydrocarbons such as ethane are important precursors to tropospheric ozone and aerosols. Using data from a global surface network and atmospheric column observations we show that the steady decline in ethane concentrations that began in the 1970s halted between 2005 and 2010 in most of the Northern Hemisphere, and has since reversed. We calculate a yearly increase in ethane emissions in the Northern Hemisphere of 0.42 (+/-0.19) Tg/yr between mid-2009 and mid-2014. The largest increases in ethane and for the shorter-lived propane are seen over the central and eastern USA, with a spatial distribution that suggests North American oil and natural gas development as the primary source of increasing emissions. By including other co-emitted oil and natural gas non-methane hydrocarbons, we estimate a Northern Hemisphere total non-methane hydrocarbon yearly emission increase of 1.2 (+/-0.8) Tg/yr. Atmospheric chemical transport modelling suggests that these emissions could augment summertime mean surface ozone by several nanomoles per mole near oil and natural gas production regions. Methane/ethane oil and natural gas emission ratios suggest a significant increase in associated methane emissions; however, this increase is inconsistent with observed leak rates in production regions and changes in methane’s global isotopic ratio. [less ▲]

Detailed reference viewed: 99 (25 ULiège)
Full Text
See detailComparison of surface and column carbon monoxide at a high altitude, a megacity and a southern hemisphere site
Té, Yao; Jeseck, Pascal; Franco, Bruno ULiege et al

Conference (2016, June 02)

Detailed reference viewed: 29 (1 ULiège)
Full Text
See detailA Reversal of Long-term Global Trends in Atmospheric Ethane and Propane from North American Oil and Natural Gas Emissions
Helmig, D.; Rossabi, S.; Hueber, J. et al

Conference (2016, May 18)

Ethane, the longest-lived and most abundant non-methane hydrocarbon (NMHC) peaked in the background atmosphere around 1970. This was followed by a ~20% reduction of the atmospheric burden and a resulting ... [more ▼]

Ethane, the longest-lived and most abundant non-methane hydrocarbon (NMHC) peaked in the background atmosphere around 1970. This was followed by a ~20% reduction of the atmospheric burden and a resulting atmospheric downward trend for the next four decades, mostly due to reduced emissions from oil and gas industries and stricter air quality controls. Here, we show that the near 40-year trend of declining global ethane halted between 2005-2010 in most of the Northern Hemisphere (NH), and that since it has reversed. The largest increases in ethane and of the shorter-lived propane are seen in the central and eastern U.S. and immediately downwind, identifying this region as the primary source of increased NMHC emissions. The spatial distribution of observed concentration increases for ethane and propane provides convincing evidence that renewed emissions are primarily associated with the growth of oil and natural gas development in North America. Using source region relationships, emission estimates for increases of co-emitted NMHCs and methane, as well as impacts on tropospheric ozone production have been developed. [less ▲]

Detailed reference viewed: 101 (8 ULiège)