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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 ULg 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 ▲]

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See detailModel Sensitivity Studies of the Decrease in Atmospheric Carbon Tetrachloride
Chipperfield, M. P.; Liang, Q.; Rigby, M. et al

in Atmospheric Chemistry & Physics Discussions (2016), 2016

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 ▲]

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See detailTen years of atmospheric methane from ground-based NDACC FTIR observations
Bader, Whitney ULg; Bovy, Benoît ULg; Conway, S. et al

in Atmospheric Chemistry & Physics Discussions (2016), 2016

Changes of atmospheric methane (CH4) since 2005 have been evaluated using Fourier Transform Infrared (FTIR) solar observations performed at ten ground-based sites, all members of the Network for Detection ... [more ▼]

Changes of atmospheric methane (CH4) since 2005 have been evaluated using Fourier Transform Infrared (FTIR) solar observations performed at ten ground-based sites, all members of the Network for Detection of Atmospheric Composition Change (NDACC). From this, we find an increase of atmospheric methane total columns that amounts to 0.31 ± 0.03 % year-1 (2-sigma level of uncertainty) for the 2005–2014 period. Comparisons with in situ methane measurements at both local and global scales show good agreement. We used the GEOS-Chem Chemical Transport Model tagged simulation that accounts for the contribution of each emission source and one sink in the total methane, simulated over the 2005–2012 time period and based on emissions inventories and transport. After regridding according to NDACC vertical layering using a conservative regridding scheme and smoothing by convolving with respective FTIR seasonal averaging kernels, the GEOS-Chem simulation shows an increase of atmospheric methane of 0.35 ± 0.03 % year-1 between 2005 and 2012, which is in agreement with NDACC measurements over the same time period (0.30 ± 0.04 % year-1, averaged over ten 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 inter-annual 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 ▲]

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See detailIntercomparison of in-situ NDIR and column FTIR measurements of CO2 at Jungfraujoch
Schibig, M. F.; Mahieu, Emmanuel ULg; 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 ▲]

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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 ▲]

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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. Papers in Open Discussion (2016), 2016

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 ▲]

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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 ▲]

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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 ▲]

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See detailOptimized approach to retrieve information on atmospheric carbonyl sulfide (OCS) above the Jungfraujoch station and change in its abundance since 1995
Lejeune, Bernard ULg; Mahieu, Emmanuel ULg; Vollmer, M. K. et al

in Journal of Quantitative Spectroscopy & Radiative Transfer (2016), 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 ▲]

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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 ULg et al

Conference (2016, June 02)

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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 ▲]

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See detailEthane rise associated with North American oil and gas exploitation
Franco, Bruno ULg; Mahieu, Emmanuel ULg; Emmons, Louisa et al

Conference (2016, May 18)

Ethane (C2H6) is mainly emitted in the atmosphere from leakage during production and transport of natural gas, biofuel consumption and biomass burning. As it shares concurrent anthropogenic emission ... [more ▼]

Ethane (C2H6) is mainly emitted in the atmosphere from leakage during production and transport of natural gas, biofuel consumption and biomass burning. As it shares concurrent anthropogenic emission sources with methane (CH4), a better understanding of the atmospheric distribution of C2H6 and any trends in its abundance can be used to better constrain the sources of CH4 from oil and gas activities. Until very recently, the C2H6 abundance in the atmosphere has been declining due to the reduction of fugitive emissions as a result of air pollution abatement measures. However, a renewal of the atmospheric C2H6 burden has been detected over North America and Europe from 2009 onwards. It is attributed to the unprecedented growth in the exploitation of shale gas and tight oil reservoirs in North America. Using time series of C2H6 abundance derived from ground-based high-resolution infrared solar absorption spectra recorded at complementary NDACC FTIR sites, we present here sharp C2H6 rises in the Northern Hemisphere, of up to 5 %/yr since 2009. Using model simulations, we show that the HTAP2 bottom-up inventories for anthropogenic emissions greatly underestimate the observed pre-increase C2H6 abundances and that they are too low by a factor two. We also evaluate new top-down emissions of C2H6 from the North American oil and gas activities, biofuel consumption and biomass burning, derived from space-borne observations of CH4 from GOSAT. We find a good agreement with the observations at the North American mid-latitudinal sites, close to regions with high drilling productivity, but an overestimation at remote sites. We also estimate that the North American C2H6 emissions have increased by 75% over the past six years (2009-2014), annihilating the benefits of more than two decades of successful anthropogenic emission reduction, and that the associated annual CH4 emissions from the North American oil and gas sector grew from 20 to 35 Tg/yr over the same period. [less ▲]

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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 Discussions (2016)

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 such 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 ▲]

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See detailUsing NDACC column measurements of carbonyl sulfide to estimate its sources and sinks
Wang; Marshall, J; Palm, M et al

in Geophysical Research Abstracts (2016, April 19), 18

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See detailEvaluating ethane and methane emissions associated with the development of oil and natural gas extraction in North America
Franco, Bruno ULg; Mahieu, Emmanuel ULg; Emmons, L. K. et al

in Environmental Research Letters (2016), 11(4), 044010

Sharp rises in the atmospheric abundance of ethane (C2H6) have been detected from 2009 onwards in the Northern Hemisphere as a result of the unprecedented growth in the exploitation of shale gas and tight ... [more ▼]

Sharp rises in the atmospheric abundance of ethane (C2H6) have been detected from 2009 onwards in the Northern Hemisphere as a result of the unprecedented growth in the exploitation of shale gas and tight oil reservoirs in North America. Using time series of C2H6 total columns derived from ground-based FTIR observations made at five selected NDACC sites, we characterize the recent C2H6 evolution and determine growth rates of ~5%/yr at mid-latitudes and of ~3%/yr at remote sites. Results from CAM-chem simulations with the HTAP2 bottom-up inventory for anthropogenic emissions are found to greatly underestimate the current C2H6 abundances. Doubling global emissions is required to reconcile the simulations and the observations prior to 2009. We further estimate that North American anthropogenic C2H6 emissions have increased from 1.6 Tg/yr in 2008 to 2.8 Tg/yr in 2014, i.e. by 75% over these six years. We also completed a second simulation with new top-down emissions of C2H6 from North American oil and gas activities, biofuel consumption and biomass burning, inferred from space-borne observations of methane (CH4) from GOSAT. In this simulation, GEOS-Chem is able to reproduce FTIR measurements at the mid-latitudinal sites, underscoring the impact of the North American oil and gas development on the current C2H6 abundance. Finally we estimate that the North American oil and gas emissions of CH4, a major greenhouse gas, grew from 20 to 35 Tg/yr over the period 2008 to 2014, in association with the recent C2H6 rise. [less ▲]

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See detailDiurnal cycle and multi-decadal trend of formaldehyde in the remote atmosphere near 46° N
Franco, Bruno ULg; Marais, Eloise A.; Bovy, Benoît ULg et al

in Atmospheric Chemistry and Physics (2016), 16

Only very few long-term records of formaldehyde (HCHO) exist that are suitable for trend analysis. Furthermore, many uncertainties remain as to its diurnal cycle, representing a large short-term ... [more ▼]

Only very few long-term records of formaldehyde (HCHO) exist that are suitable for trend analysis. Furthermore, many uncertainties remain as to its diurnal cycle, representing a large short-term variability superimposed on seasonal and inter-annual variations that should be accounted for when comparing ground-based observations to e.g., model results. In this study, we derive a multi-decadal time series (January 1988 – June 2015) of HCHO total columns from ground-based high-resolution Fourier transform infrared (FTIR) solar spectra recorded at the high-altitude station of Jungfraujoch (Swiss Alps, 46.5° N, 8.0° E, 3580 m a.s.l.), allowing for the characterization of the mid-latitudinal atmosphere for background conditions. First we investigate the HCHO diurnal variation, peaking around noontime and mainly driven by the intra-day insolation modulation and methane (CH4) oxidation. We also characterize quantitatively the diurnal cycles by adjusting a parametric model to the observations, which links the daytime to the HCHO columns according to the monthly intra-day regimes. It is then employed to scale all the individual FTIR measurements on a given daytime in order to remove the effect of the intra-day modulation for improving the trend determination and the comparison with HCHO columns simulated by the state-of-the-art chemical transport model GEOS-Chem v9-02. Such a parametric model will be useful to scale the Jungfraujoch HCHO columns on satellite overpass times in the framework of future calibration/validation efforts of space borne sensors. GEOS-Chem sensitivity tests suggest then that the seasonal and inter-annual HCHO column variations above Jungfraujoch are predominantly led by the atmospheric CH4 oxidation, with a maximum contribution of 25 % from the anthropogenic non-methane volatile organic compound precursors during wintertime. Finally, trend analysis of the so-scaled 27-year FTIR time series reveals a long-term evolution of the HCHO columns in the remote troposphere to be related with the atmospheric CH4 fluctuations and the short-term OH variability: +2.9 %/yr between 1988 and 1995, -3.7 %/yr over 1996-2002 and +0.8/% yr from 2003 onwards. [less ▲]

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See detailStratospheric aerosol - Observations, processes, and impact on climate
Kremser, Stefanie; Thomason, Larry W.; von Hobe, Marc et al

in Reviews of Geophysics (Washington, D.C. : 1985) (2016)

Interest in stratospheric aerosol and its role in climate has increased over the last decade due to the observed increase in stratospheric aerosol since 2000 and the potential for changes in the sulfur ... [more ▼]

Interest in stratospheric aerosol and its role in climate has increased over the last decade due to the observed increase in stratospheric aerosol since 2000 and the potential for changes in the sulfur cycle induced by climate change. This review provides an overview about the advances in stratospheric aerosol research since the last comprehensive assessment of stratospheric aerosol was published in 2006. A crucial development since 2006 is the substantial improvement in the agreement between in situ and space-based inferences of stratospheric aerosol properties during volcanically quiescent periods. Furthermore, new measurement systems and techniques, both in situ and space-based, have been developed for measuring physical aerosol properties with greater accuracy and for characterizing aerosol composition. However, these changes induce challenges to constructing a long-term stratospheric aerosol climatology. Currently, changes in stratospheric aerosol levels less than 20% cannot be confidently quantified. The volcanic signals tend to mask any non-volcanically driven change, making them difficult to understand. While the role of carbonyl sulfide (OCS) as a substantial and relatively constant source of stratospheric sulfur has been confirmed by new observations and model simulations, large uncertainties remain with respect to the contribution from anthropogenic sulfur dioxide (SO2) emissions. New evidence has been provided that stratospheric aerosol can also contain small amounts of non-sulfate matter such as black carbon and organics. Chemistry-climate models have substantially increased in quantity and sophistication. In many models the implementation of stratospheric aerosol processes is coupled to radiation and/or stratospheric chemistry modules to account for relevant feedback processes. [less ▲]

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See detailRetrieval of HCFC-142b (CH3CClF2) from ground-based high-resolution infrared solar spectra: Atmospheric increase since 1989 and comparison with surface and satellite measurements
Mahieu, Emmanuel ULg; Lejeune, Bernard ULg; Bovy, Benoît ULg et al

in Journal of Quantitative Spectroscopy & Radiative Transfer (2016)

We have developed an approach for retrieving HCFC-142b (CH3CClF2) from ground-based high-resolution infrared solar spectra, using its ν7 band Q branch in the 900–906 cm-1 interval. Interferences by HNO3 ... [more ▼]

We have developed an approach for retrieving HCFC-142b (CH3CClF2) from ground-based high-resolution infrared solar spectra, using its ν7 band Q branch in the 900–906 cm-1 interval. Interferences by HNO3, CO2 and H2O have to be accounted for. Application of this approach to observations recorded within the framework of long-term monitoring activities carried out at the northern mid-latitude, high-altitude Jungfraujoch station in Switzerland (46.5°N, 8.0°E, 3580 m above sea level) has provided a total column times series spanning the 1989 to mid-2015 time period. A fit to the HCFC-142b daily mean total column time series shows a statistically-significant long-term trend of (1.23±0.08×1013 molec cm-2) per year from 2000 to 2010, at the 2-σ confidence level. This corresponds to a significant atmospheric accumulation of (0.94±0.06) ppt (1 ppt=10-12) per year for the mean tropospheric mixing ratio, at the 2−σ confidence level. Over the subsequent time period (2010–2014), we note a significant slowing down in the HCFC-142b buildup. Our ground-based FTIR (Fourier Transform Infrared) results are compared with relevant data sets derived from surface in situ measurements at the Mace Head and Jungfraujoch sites of the AGAGE (Advanced Global Atmospheric Gases Experiment) network and from occultation measurements by the ACE-FTS (Atmospheric Chemistry Experiment-Fourier Transform Spectrometer) instrument on-board the SCISAT satellite. [less ▲]

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See detailReversal of Long-Term Trends in Ethane Identified from the Global Atmosphere Watch Reactive Gases Measurement Network
Helmig, Detlev; Buchmann, Brigitte; Carpenter, Lucy et al

Poster (2016, March 02)

Reactive gases play an important role in climate and air pollution issues. They control the self-cleansing capability of the troposphere, contribute to air pollution and acid deposition, regulate the ... [more ▼]

Reactive gases play an important role in climate and air pollution issues. They control the self-cleansing capability of the troposphere, contribute to air pollution and acid deposition, regulate the lifetimes and provide tracers for deciphering sources and sinks for greenhouse gases. Within GAW, the focus is placed on long-term, high-quality observations of ozone (O3), carbon monoxide (CO), volatile organic compounds (VOC), nitrogen oxides (NOx), and sulfur dioxide (SO2). More than 100 stations worldwide carry out reactive gases measurements with data reported to two World Data Centers. The reactive gases program in GAW cooperates The WMO GAW Reactive Gases Program with regional networks and other global monitoring initiatives in order to attain a complete picture of the tropospheric chemical composition. Observations are being made by in-situ monitoring, measurements from commercial routine air-crafts (e.g. IAGOS), column observations, and from flask sampling networks. Quality control and coordination of measurements between participating stations are a primary emphasis. GAW reactive gases data in rapid delivery mode are used to evaluate operational atmospheric composition forecasts in the EU Copernicus Atmospheric Monitoring Service. Oversight of the program is provided by GAW-WMO coordinated Reactive Gases Scientific Advisory Committee (RG-SAG). [less ▲]

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See detailTowards understanding the variability in biospheric CO2 fluxes: using FTIR spectrometry and a chemical transport model to investigate the sources and sinks of carbonyl sulfide and its link to CO2
Wang, Y.; Deutscher, N. M.; Palm, M. et al

in Atmospheric Chemistry and Physics (2016), 16

Understanding carbon dioxide (CO2) biospheric processes is of great importance because the terrestrial exchange drives the seasonal and interannual variability of CO2 in the atmosphere. Atmospheric ... [more ▼]

Understanding carbon dioxide (CO2) biospheric processes is of great importance because the terrestrial exchange drives the seasonal and interannual variability of CO2 in the atmosphere. Atmospheric inversions based on CO2 concentration measurements alone can only determine net biosphere fluxes, but not differentiate between photosynthesis (uptake) and respiration (production). Carbonyl sulfide (OCS) could provide an important additional constraint: it is also taken up by plants during photosynthesis but not emitted during respiration, and therefore is a potential means to differentiate between these processes. Solar absorption Fourier Transform InfraRed (FTIR) spectrometry allows for the retrievals of the atmospheric concentrations of both CO2 and OCS from measured solar absorption spectra. Here, we investigate co-located and quasi-simultaneous FTIR measurements of OCS and CO2 performed at five selected sites located in the Northern Hemisphere. These measurements are compared to simulations of OCS and CO2 using a chemical transport model (GEOS-Chem). The coupled biospheric fluxes of OCS and CO2 from the simple biosphere model (SiB) are used in the study. The CO2 simulation with SiB fluxes agrees with the measurements well, while the OCS simulation reproduced a weaker drawdown than FTIR measurements at selected sites, and a smaller latitudinal gradient in the Northern Hemisphere during growing season when comparing with HIPPO (HIAPER Pole-to-Pole Observations) data spanning both hemispheres. An offset in the timing of the seasonal cycle minimum between SiB simulation and measurements is also seen. Using OCS as a photosynthesis proxy can help to understand how the biospheric processes are reproduced in models and to further understand the carbon cycle in the real world. [less ▲]

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