Articles | Volume 16, issue 16
https://doi.org/10.5194/acp-16-10469-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-16-10469-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
19 Aug 2016
Research article |
| 19 Aug 2016
In situ observations of the isotopic composition of methane at the Cabauw tall tower site
Utrecht University, Institute for Marine and Atmospheric Research
Utrecht, Utrecht, the Netherlands
Simon Eyer
Empa, Laboratory for Air Pollution/Environmental Technology,
Dübendorf, Switzerland
Carina van der Veen
Utrecht University, Institute for Marine and Atmospheric Research
Utrecht, Utrecht, the Netherlands
Maria E. Popa
Utrecht University, Institute for Marine and Atmospheric Research
Utrecht, Utrecht, the Netherlands
Béla Tuzson
Empa, Laboratory for Air Pollution/Environmental Technology,
Dübendorf, Switzerland
Guillaume Monteil
Utrecht University, Institute for Marine and Atmospheric Research
Utrecht, Utrecht, the Netherlands
now at: Department of Physical Geography and Ecosystem Science, Lund
University, Lund, Sweden
Sander Houweling
Utrecht University, Institute for Marine and Atmospheric Research
Utrecht, Utrecht, the Netherlands
Eliza Harris
Empa, Laboratory for Air Pollution/Environmental Technology,
Dübendorf, Switzerland
Dominik Brunner
Empa, Laboratory for Air Pollution/Environmental Technology,
Dübendorf, Switzerland
Hubertus Fischer
University of Bern, Climate and Environmental Physics, Bern,
Switzerland
Giulia Zazzeri
Royal Holloway University of London, Department of Earth
Sciences, Egham, UK
David Lowry
Royal Holloway University of London, Department of Earth
Sciences, Egham, UK
Euan G. Nisbet
Royal Holloway University of London, Department of Earth
Sciences, Egham, UK
Willi A. Brand
Max Planck Institute for Biogeochemistry, Jena, Germany
Jaroslav M. Necki
Environmental Physics Group, Faculty of Physics and Applied Computer
Science, AGH University of Science and Technology, Krakow, Poland
Lukas Emmenegger
Empa, Laboratory for Air Pollution/Environmental Technology,
Dübendorf, Switzerland
Joachim Mohn
Empa, Laboratory for Air Pollution/Environmental Technology,
Dübendorf, Switzerland
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Malika Menoud, Carina van der Veen, Jaroslaw Necki, Jakub Bartyzel, Barbara Szénási, Mila Stanisavljević, Isabelle Pison, Philippe Bousquet, and Thomas Röckmann
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Xinyi Lu, Stephen J. Harris, Rebecca E. Fisher, James L. France, Euan G. Nisbet, David Lowry, Thomas Röckmann, Carina van der Veen, Malika Menoud, Stefan Schwietzke, and Bryce F. J. Kelly
Atmos. Chem. Phys., 21, 10527–10555, https://doi.org/10.5194/acp-21-10527-2021, https://doi.org/10.5194/acp-21-10527-2021, 2021
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Max Thomas, Johannes C. Laube, Jan Kaiser, Samuel Allin, Patricia Martinerie, Robert Mulvaney, Anna Ridley, Thomas Röckmann, William T. Sturges, and Emmanuel Witrant
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Hossein Maazallahi, Julianne M. Fernandez, Malika Menoud, Daniel Zavala-Araiza, Zachary D. Weller, Stefan Schwietzke, Joseph C. von Fischer, Hugo Denier van der Gon, and Thomas Röckmann
Atmos. Chem. Phys., 20, 14717–14740, https://doi.org/10.5194/acp-20-14717-2020, https://doi.org/10.5194/acp-20-14717-2020, 2020
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Joram J. D. Hooghiem, Maria Elena Popa, Thomas Röckmann, Jens-Uwe Grooß, Ines Tritscher, Rolf Müller, Rigel Kivi, and Huilin Chen
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Wildfires release a large quantity of pollutants that can reach the stratosphere through pyro-convection events. In September 2017, a stratospheric plume was accidentally sampled during balloon soundings in northern Finland. The source of the plume was identified to be wildfire smoke based on in situ measurements of carbon monoxide (CO) and stable isotope analysis of CO. Furthermore, the age of the plume was estimated using backwards transport modelling to be ~24 d, with its origin in Canada.
Alina Fiehn, Julian Kostinek, Maximilian Eckl, Theresa Klausner, Michał Gałkowski, Jinxuan Chen, Christoph Gerbig, Thomas Röckmann, Hossein Maazallahi, Martina Schmidt, Piotr Korbeń, Jarosław Neçki, Pawel Jagoda, Norman Wildmann, Christian Mallaun, Rostyslav Bun, Anna-Leah Nickl, Patrick Jöckel, Andreas Fix, and Anke Roiger
Atmos. Chem. Phys., 20, 12675–12695, https://doi.org/10.5194/acp-20-12675-2020, https://doi.org/10.5194/acp-20-12675-2020, 2020
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A severe reduction of greenhouse gas emissions is necessary to fulfill the Paris Agreement. We use aircraft- and ground-based in situ observations of trace gases and wind speed from two flights over the Upper Silesian Coal Basin, Poland, for independent emission estimation. The derived methane emission estimates are within the range of emission inventories, carbon dioxide estimates are in the lower range and carbon monoxide emission estimates are slightly higher than emission inventory values.
Jordi Vilà-Guerau de Arellano, Patrizia Ney, Oscar Hartogensis, Hugo de Boer, Kevin van Diepen, Dzhaner Emin, Geiske de Groot, Anne Klosterhalfen, Matthias Langensiepen, Maria Matveeva, Gabriela Miranda-García, Arnold F. Moene, Uwe Rascher, Thomas Röckmann, Getachew Adnew, Nicolas Brüggemann, Youri Rothfuss, and Alexander Graf
Biogeosciences, 17, 4375–4404, https://doi.org/10.5194/bg-17-4375-2020, https://doi.org/10.5194/bg-17-4375-2020, 2020
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The CloudRoots field experiment has obtained an open comprehensive observational data set that includes soil, plant, and atmospheric variables to investigate the interactions between a heterogeneous land surface and its overlying atmospheric boundary layer, including the rapid perturbations of clouds in evapotranspiration. Our findings demonstrate that in order to understand and represent diurnal variability, we need to measure and model processes from the leaf to the landscape scales.
Johannes C. Laube, Emma C. Leedham Elvidge, Karina E. Adcock, Bianca Baier, Carl A. M. Brenninkmeijer, Huilin Chen, Elise S. Droste, Jens-Uwe Grooß, Pauli Heikkinen, Andrew J. Hind, Rigel Kivi, Alexander Lojko, Stephen A. Montzka, David E. Oram, Steve Randall, Thomas Röckmann, William T. Sturges, Colm Sweeney, Max Thomas, Elinor Tuffnell, and Felix Ploeger
Atmos. Chem. Phys., 20, 9771–9782, https://doi.org/10.5194/acp-20-9771-2020, https://doi.org/10.5194/acp-20-9771-2020, 2020
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We demonstrate that AirCore technology, which is based on small low-cost balloons, can provide access to trace gas measurements such as CFCs at ultra-low abundances. This is a new way to quantify ozone-depleting, and related, substances in the stratosphere, which is largely inaccessible to aircraft. We show two potential uses: (a) tracking the stratospheric circulation, which is predicted to change, and (b) assessing three common meteorological reanalyses driving a global stratospheric model.
Getachew Agmuas Adnew, Thijs L. Pons, Gerbrand Koren, Wouter Peters, and Thomas Röckmann
Biogeosciences, 17, 3903–3922, https://doi.org/10.5194/bg-17-3903-2020, https://doi.org/10.5194/bg-17-3903-2020, 2020
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We measured the effect of photosynthesis, the largest flux in the carbon cycle, on the triple oxygen isotope composition of atmospheric CO2 at the leaf level during gas exchange using three plant species. The main factors that limit the impact of land vegetation on the triple oxygen isotope composition of atmospheric CO2 are identified, characterized and discussed. The effect of photosynthesis on the isotopic composition of CO2 is commonly quantified as discrimination (ΔA).
Jia Chen, Florian Dietrich, Hossein Maazallahi, Andreas Forstmaier, Dominik Winkler, Magdalena E. G. Hofmann, Hugo Denier van der Gon, and Thomas Röckmann
Atmos. Chem. Phys., 20, 3683–3696, https://doi.org/10.5194/acp-20-3683-2020, https://doi.org/10.5194/acp-20-3683-2020, 2020
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We demonstrate for the first time that large festivals can be significant methane sources, though they are not included in emission inventories. We combined in situ measurements with a Gaussian plume model to determine the Oktoberfest emissions and show that they are not due solely to human biogenic emissions, but are instead primarily fossil fuel related. Our study provides the foundation to develop reduction policies for such events and new pathways to mitigate fossil fuel methane emissions.
Stefan Lossow, Charlotta Högberg, Farahnaz Khosrawi, Gabriele P. Stiller, Ralf Bauer, Kaley A. Walker, Sylvia Kellmann, Andrea Linden, Michael Kiefer, Norbert Glatthor, Thomas von Clarmann, Donal P. Murtagh, Jörg Steinwagner, Thomas Röckmann, and Roland Eichinger
Atmos. Meas. Tech., 13, 287–308, https://doi.org/10.5194/amt-13-287-2020, https://doi.org/10.5194/amt-13-287-2020, 2020
Marco de Bruine, Maarten Krol, Jordi Vilà-Guerau de Arellano, and Thomas Röckmann
Geosci. Model Dev., 12, 5177–5196, https://doi.org/10.5194/gmd-12-5177-2019, https://doi.org/10.5194/gmd-12-5177-2019, 2019
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An aerosol scheme with multiple aerosol species is introduced in the Dutch Atmospheric Large-Eddy Simulation model (DALES) and focused to simulate the feedback of aerosol–cloud interaction (ACI) on the aerosol population. Cloud aerosol processing is found to be sensitive to the numerical method, while removal by precipitation is more stable. How ACI increases or decreases the mean aerosol size depends on the balance between the evaporation of clouds/rain and ultimate removal by precipitation.
Iris N. Dekker, Sander Houweling, Sudhanshu Pandey, Maarten Krol, Thomas Röckmann, Tobias Borsdorff, Jochen Landgraf, and Ilse Aben
Atmos. Chem. Phys., 19, 3433–3445, https://doi.org/10.5194/acp-19-3433-2019, https://doi.org/10.5194/acp-19-3433-2019, 2019
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During November 2017, very high pollution levels were measured in the northern part of India. In this study, satellite (TROPOMI) data and model (WRF) data on carbon monoxide (CO) are studied to investigate the main sources of the CO pollution over the Indo-Gangetic Plain. We found that residential and commercial combustion was a much more important source of CO than the post-monsoon crop burning during this period. Meteorology was found important in the accumulation and ventilation of CO.
Dušan Materić, Elke Ludewig, Kangming Xu, Thomas Röckmann, and Rupert Holzinger
The Cryosphere, 13, 297–307, https://doi.org/10.5194/tc-13-297-2019, https://doi.org/10.5194/tc-13-297-2019, 2019
Marco de Bruine, Maarten Krol, Twan van Noije, Philippe Le Sager, and Thomas Röckmann
Geosci. Model Dev., 11, 1443–1465, https://doi.org/10.5194/gmd-11-1443-2018, https://doi.org/10.5194/gmd-11-1443-2018, 2018
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Precipitation evaporation (PE) and subsequent aerosol resuspension (AR) are currently ignored or implemented only crudely in GCMs. This research introduces PE to Earth system model EC-Earth and explores ways to treat AR and the impact on global aerosol burden. Simple 1:1 scaling of AR with PE leads to an increase (+8 to 15.9 %). Taking into account raindrop size distribution and/or accounting for in-rain aerosol processing decreases aerosol burden -1.5 to 6.2 % and -10 to -11 %, respectively.
Karina E. Adcock, Claire E. Reeves, Lauren J. Gooch, Emma C. Leedham Elvidge, Matthew J. Ashfold, Carl A. M. Brenninkmeijer, Charles Chou, Paul J. Fraser, Ray L. Langenfelds, Norfazrin Mohd Hanif, Simon O'Doherty, David E. Oram, Chang-Feng Ou-Yang, Siew Moi Phang, Azizan Abu Samah, Thomas Röckmann, William T. Sturges, and Johannes C. Laube
Atmos. Chem. Phys., 18, 4737–4751, https://doi.org/10.5194/acp-18-4737-2018, https://doi.org/10.5194/acp-18-4737-2018, 2018
Emma C. Leedham Elvidge, Harald Bönisch, Carl A. M. Brenninkmeijer, Andreas Engel, Paul J. Fraser, Eileen Gallacher, Ray Langenfelds, Jens Mühle, David E. Oram, Eric A. Ray, Anna R. Ridley, Thomas Röckmann, William T. Sturges, Ray F. Weiss, and Johannes C. Laube
Atmos. Chem. Phys., 18, 3369–3385, https://doi.org/10.5194/acp-18-3369-2018, https://doi.org/10.5194/acp-18-3369-2018, 2018
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Chemical species measured in stratospheric air can be used as proxies for stratospheric circulation changes which cannot be measured directly. A range of tracers is important to understand changing stratospheric dynamics. We demonstrate the suitability of PFCs and HFCs as tracers and support recent work that reduces the current stratospheric lifetime of SF6. Updates to policy-relevant parameters (e.g. stratospheric lifetime) linked to this change are provided for O3-depleting substances.
Taku Umezawa, Carl A. M. Brenninkmeijer, Thomas Röckmann, Carina van der Veen, Stanley C. Tyler, Ryo Fujita, Shinji Morimoto, Shuji Aoki, Todd Sowers, Jochen Schmitt, Michael Bock, Jonas Beck, Hubertus Fischer, Sylvia E. Michel, Bruce H. Vaughn, John B. Miller, James W. C. White, Gordon Brailsford, Hinrich Schaefer, Peter Sperlich, Willi A. Brand, Michael Rothe, Thomas Blunier, David Lowry, Rebecca E. Fisher, Euan G. Nisbet, Andrew L. Rice, Peter Bergamaschi, Cordelia Veidt, and Ingeborg Levin
Atmos. Meas. Tech., 11, 1207–1231, https://doi.org/10.5194/amt-11-1207-2018, https://doi.org/10.5194/amt-11-1207-2018, 2018
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Isotope measurements are useful for separating different methane sources. However, the lack of widely accepted standards and calibration methods for stable carbon and hydrogen isotopic ratios of methane in air has caused significant measurement offsets among laboratories. We conducted worldwide interlaboratory comparisons, surveyed the literature and assessed them systematically. This study may be of help in future attempts to harmonize data sets of isotopic composition of atmospheric methane.
Iris N. Dekker, Sander Houweling, Ilse Aben, Thomas Röckmann, Maarten Krol, Sara Martínez-Alonso, Merritt N. Deeter, and Helen M. Worden
Atmos. Chem. Phys., 17, 14675–14694, https://doi.org/10.5194/acp-17-14675-2017, https://doi.org/10.5194/acp-17-14675-2017, 2017
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This study estimates carbon monoxide emissions from the city of Madrid using MOPITT satellite data. There are two methods used and reviewed in this paper: a method that can only estimate a trend in the emission and a newly developed method that also includes model data from WRF to quantify the emissions. We find Madrid CO emissions to be lower by 48 % for 2002 and by 17 % for 2006 compared with the EdgarV4.2 emission inventory, but uncertainty (20 to 50 %) remains.
Carl Meusinger, Ulrike Dusek, Stephanie M. King, Rupert Holzinger, Thomas Rosenørn, Peter Sperlich, Maxime Julien, Gerald S. Remaud, Merete Bilde, Thomas Röckmann, and Matthew S. Johnson
Atmos. Chem. Phys., 17, 6373–6391, https://doi.org/10.5194/acp-17-6373-2017, https://doi.org/10.5194/acp-17-6373-2017, 2017
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Isotope studies can constrain budgets of secondary organic aerosol (SOA) that is pivotal to air pollution and climate. SOA from α-pinene ozonolysis was found to be enriched in 13C relative to the precursor. The observed difference in 13C between the gas and particle phases may arise from isotope-dependent changes in branching ratios. Alternatively, some gas-phase products involve carbon atoms from highly enriched and depleted sites, giving a non-kinetic origin to the observed fractionations.
Célia J. Sapart, Natalia Shakhova, Igor Semiletov, Joachim Jansen, Sönke Szidat, Denis Kosmach, Oleg Dudarev, Carina van der Veen, Matthias Egger, Valentine Sergienko, Anatoly Salyuk, Vladimir Tumskoy, Jean-Louis Tison, and Thomas Röckmann
Biogeosciences, 14, 2283–2292, https://doi.org/10.5194/bg-14-2283-2017, https://doi.org/10.5194/bg-14-2283-2017, 2017
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The Arctic Ocean, especially the Siberian shelves, overlays large areas of subsea permafrost that is degrading. We show that methane with a biogenic origin is emitted from this permafrost. At locations where bubble plumes have been observed, methane can escape oxidation in the surface sediment and rapidly migrate through the very shallow water column of this region to escape to the atmosphere, generating a positive radiative feedback.
Markella Prokopiou, Patricia Martinerie, Célia J. Sapart, Emmanuel Witrant, Guillaume Monteil, Kentaro Ishijima, Sophie Bernard, Jan Kaiser, Ingeborg Levin, Thomas Blunier, David Etheridge, Ed Dlugokencky, Roderik S. W. van de Wal, and Thomas Röckmann
Atmos. Chem. Phys., 17, 4539–4564, https://doi.org/10.5194/acp-17-4539-2017, https://doi.org/10.5194/acp-17-4539-2017, 2017
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Nitrous oxide is the third most important anthropogenic greenhouse gas with an increasing mole fraction. To understand its natural and anthropogenic sources
we employ isotope measurements. Results show that while the N2O mole fraction increases, its heavy isotope content decreases. The isotopic changes observed underline the dominance of agricultural emissions especially at the early part of the record, whereas in the later decades the contribution from other anthropogenic sources increases.
Ulrike Dusek, Regina Hitzenberger, Anne Kasper-Giebl, Magdalena Kistler, Harro A. J. Meijer, Sönke Szidat, Lukas Wacker, Rupert Holzinger, and Thomas Röckmann
Atmos. Chem. Phys., 17, 3233–3251, https://doi.org/10.5194/acp-17-3233-2017, https://doi.org/10.5194/acp-17-3233-2017, 2017
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Measurements of the radioactive carbon isotope 14C allow to identify the sources of aerosol carbon. We report an extensive 14C source apportionment record in the Netherlands with samples covering a whole year. We discovered that long-range transport has a large influence on aerosol carbon levels. Fossil fuel carbon is least influenced by long-range transport and more regional in origin. Biomass burning seems to be a minor source of aerosol carbon in the Netherlands.
Bastiaan Jonkheid, Thomas Röckmann, Norbert Glatthor, Christof Janssen, Gabriele Stiller, and Thomas von Clarmann
Atmos. Meas. Tech., 9, 6069–6079, https://doi.org/10.5194/amt-9-6069-2016, https://doi.org/10.5194/amt-9-6069-2016, 2016
Dorota Janina Mrozek, Carina van der Veen, Magdalena E. G. Hofmann, Huilin Chen, Rigel Kivi, Pauli Heikkinen, and Thomas Röckmann
Atmos. Meas. Tech., 9, 5607–5620, https://doi.org/10.5194/amt-9-5607-2016, https://doi.org/10.5194/amt-9-5607-2016, 2016
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Stratospheric Air Sub-sampler (SAS) is a device to collect and to store the stratospheric profile of air collected with an AirCore (Karion et al., 2010) in numerous sub-samples. The sub-samples (each of 25 mL at ambient temperature and pressure) can be later introduced to the continuous flow systems to measure for example the isotopic composition of CO2. The performance of the coupled system is demonstrated for a set of air samples from an AirCore flight in November 2014 near Sodankylä, Finland.
Beatriz Sayuri Oyama, Maria de Fátima Andrade, Pierre Herckes, Ulrike Dusek, Thomas Röckmann, and Rupert Holzinger
Atmos. Chem. Phys., 16, 14397–14408, https://doi.org/10.5194/acp-16-14397-2016, https://doi.org/10.5194/acp-16-14397-2016, 2016
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Vehicular emissions have a strong impact on air pollution in big cities; hence, the study was performed in São Paulo city, where light- (LDVs) and heavy-duty vehicles (HDVs) run on different fuels. We find that organic aerosol emission from LDVs and HDVs is a complex process involving oxidation of fuel constituents, NOx chemistry, and condensation of unburned fuel hydrocarbons on new or existing particles. The obtained emission patterns can be used to study processing of young aerosol in Brazil.
Matthias Egger, Peter Kraal, Tom Jilbert, Fatimah Sulu-Gambari, Célia J. Sapart, Thomas Röckmann, and Caroline P. Slomp
Biogeosciences, 13, 5333–5355, https://doi.org/10.5194/bg-13-5333-2016, https://doi.org/10.5194/bg-13-5333-2016, 2016
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By combining detailed geochemical analyses with diagenetic modeling, we provide new insights into how methane dynamics may strongly overprint burial records of iron, sulfur and phosphorus in marine systems subject to changes in organic matter loading or water column salinity. A better understanding of these processes will improve our ability to read ancient sediment records and thus to predict the potential consequences of global warming and human-enhanced inputs of nutrients to the ocean.
Peter Sperlich, Nelly A. M. Uitslag, Jürgen M. Richter, Michael Rothe, Heike Geilmann, Carina van der Veen, Thomas Röckmann, Thomas Blunier, and Willi A. Brand
Atmos. Meas. Tech., 9, 3717–3737, https://doi.org/10.5194/amt-9-3717-2016, https://doi.org/10.5194/amt-9-3717-2016, 2016
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Isotope measurements in atmospheric CH4 are performed since more than 3 decades. However, standard gases to harmonize global measurements are not available to this day. We designed two methods to calibrate a suite of 8 CH4 gases with a wide range in isotopic composition to the VPDB and VSMOW scales with high precision and accuracy. Synthetic air mixtures with ~2 ppm of calibrated CH4 can be provided to the community by the ISOLAB of the Max Planck Institute for Biogeochemistry in Jena, Germany.
Sudhanshu Pandey, Sander Houweling, Maarten Krol, Ilse Aben, Frédéric Chevallier, Edward J. Dlugokencky, Luciana V. Gatti, Emanuel Gloor, John B. Miller, Rob Detmers, Toshinobu Machida, and Thomas Röckmann
Atmos. Chem. Phys., 16, 5043–5062, https://doi.org/10.5194/acp-16-5043-2016, https://doi.org/10.5194/acp-16-5043-2016, 2016
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This study investigates the constraint provided by measurements of Xratio (XCH4/XCO2) from space on surface fluxes of CH4 and CO2. We apply the ratio inversion method described in Pandey et al. (2015) to Xratio retrievals from the GOSAT with the TM5-4DVAR inverse modeling system, to constrain the surface fluxes of CH4 and CO2 for 2009 and 2010. The results are compared to proxy CH4 inversions using model-derived-XCO2 mixing ratios from CarbonTracker and MACC.
S. Eyer, B. Tuzson, M. E. Popa, C. van der Veen, T. Röckmann, M. Rothe, W. A. Brand, R. Fisher, D. Lowry, E. G. Nisbet, M. S. Brennwald, E. Harris, C. Zellweger, L. Emmenegger, H. Fischer, and J. Mohn
Atmos. Meas. Tech., 9, 263–280, https://doi.org/10.5194/amt-9-263-2016, https://doi.org/10.5194/amt-9-263-2016, 2016
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We present a newly developed field-deployable, autonomous platform simultaneously measuring the three most abundant isotopologues of methane using mid-infrared laser absorption spectroscopy.
The instrument consists of a compact quantum cascade laser absorption spectrometer (QCLAS) coupled to a preconcentration unit, called TRace gas EXtractor (TREX).
The performance of this new in situ technique was investigated during a 2-week measurement campaign and compared to other techniques.
N. Bândă, M. Krol, M. van Weele, T. van Noije, P. Le Sager, and T. Röckmann
Atmos. Chem. Phys., 16, 195–214, https://doi.org/10.5194/acp-16-195-2016, https://doi.org/10.5194/acp-16-195-2016, 2016
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We quantify the processes responsible for methane growth rate variability in the period 1990 to 1995, a period with variations in climate and radiation due to the Pinatubo eruption. We find significant contributions from changes in the methane emission from wetlands, and in the methane removal by OH caused by stratospheric aerosols, by the decrease in temperature and water vapour, by stratospheric ozone depletion and by changes in emissions of CO and NMVOC.
S. Walter, A. Kock, T. Steinhoff, B. Fiedler, P. Fietzek, J. Kaiser, M. Krol, M. E. Popa, Q. Chen, T. Tanhua, and T. Röckmann
Biogeosciences, 13, 323–340, https://doi.org/10.5194/bg-13-323-2016, https://doi.org/10.5194/bg-13-323-2016, 2016
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Oceans are a source of H2, an indirect greenhouse gas. Measurements constraining the temporal and spatial patterns of oceanic H2 emissions are sparse and although H2 is assumed to be produced mainly biologically, direct evidence for biogenic marine production was lacking. By analyzing the H2 isotopic composition (δD) we were able to constrain the global H2 budget in more detail, verify biogenic production and point to additional sources. We also showed that current models are reasonably working.
S. L. Pathirana, C. van der Veen, M. E. Popa, and T. Röckmann
Atmos. Meas. Tech., 8, 5315–5324, https://doi.org/10.5194/amt-8-5315-2015, https://doi.org/10.5194/amt-8-5315-2015, 2015
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CO is established as an important indirect greenhouse gas, as it is the major sink for the OH∙. We have developed a fully automated system for the determination of δ13C and δ18O in atmospheric CO. The blank signal of the Schütze reagent is 1-3 % of the typical sample size. The repeatability is 0.1 ‰ for δ13C and 0.2 ‰ for δ18O. The analytical repeatability for the mole fraction is ~0.7 nmol mol-1 for 100 mL of ambient air (185.4 nmol mol-1 of CO). A single measurement is performed in 18 min.
Q. Chen, M. E. Popa, A. M. Batenburg, and T. Röckmann
Atmos. Chem. Phys., 15, 13003–13021, https://doi.org/10.5194/acp-15-13003-2015, https://doi.org/10.5194/acp-15-13003-2015, 2015
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We investigated soil production and uptake of H2 and associated isotope effects. Uptake and emission of H2 occurred simultaneously at all sampling sites, with strongest emission where N2 fixing legume was present. The fractionation constant during soil uptake was about 0.945 and it did not show positive correlation with deposition velocity. The isotopic composition of H2 emitted from soil with legume was about -530‰, which is less deuterium-depleted than isotope equilibrium between H2O and H2.
S. Pandey, S. Houweling, M. Krol, I. Aben, and T. Röckmann
Atmos. Chem. Phys., 15, 8615–8629, https://doi.org/10.5194/acp-15-8615-2015, https://doi.org/10.5194/acp-15-8615-2015, 2015
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This study attempts to determine the feasibility of a new assimilation method of satellite measurements of CH4 and CO2 for optimization of their surface fluxes in a synthetic environment. Instead of their absolute concentrations, we assimilate the ratios of their concentrations (CH4/CO2) in our inversion. Doing so helps us to reduce the effect of atmospheric scattering on the measurements in our system. However, assimilation of the ratios makes the inversion non-linear.
K. Ishijima, M. Takigawa, K. Sudo, S. Toyoda, N. Yoshida, T. Röckmann, J. Kaiser, S. Aoki, S. Morimoto, S. Sugawara, and T. Nakazawa
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-15-19947-2015, https://doi.org/10.5194/acpd-15-19947-2015, 2015
Revised manuscript not accepted
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We developed an atmospheric N2O isotopocule model based on a chemistry-coupled atmospheric general circulation model and a simple method to optimize the model, and estimated the isotopic signatures of surface sources at the hemispheric scale. Data obtained from ground-based observations, measurements of firn air, and balloon and aircraft flights were used to optimize the long-term trends, interhemispheric gradients, and photolytic fractionation, respectively, in the model.
S. J. Allin, J. C. Laube, E. Witrant, J. Kaiser, E. McKenna, P. Dennis, R. Mulvaney, E. Capron, P. Martinerie, T. Röckmann, T. Blunier, J. Schwander, P. J. Fraser, R. L. Langenfelds, and W. T. Sturges
Atmos. Chem. Phys., 15, 6867–6877, https://doi.org/10.5194/acp-15-6867-2015, https://doi.org/10.5194/acp-15-6867-2015, 2015
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Stratospheric ozone protects life on Earth from harmful UV-B radiation. Chlorofluorocarbons (CFCs) are man-made compounds which act to destroy this barrier.
This paper presents (1) the first measurements of the stratospheric δ(37Cl) of CFCs -11 and -113; (2) the first quantification of long-term trends in the tropospheric δ(37Cl) of CFCs -11, -12 and -113.
This study provides a better understanding of source and sink processes associated with these destructive compounds.
F. A. Stap, O. P. Hasekamp, and T. Röckmann
Atmos. Meas. Tech., 8, 1287–1301, https://doi.org/10.5194/amt-8-1287-2015, https://doi.org/10.5194/amt-8-1287-2015, 2015
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We present the capability of an aerosol retrieval algorithm, intended for multi-angle, multi-wavelength photopolarimetric measurements, to intrinsically screen for sub-pixel liquid water cloud contamination.
The screening is based on goodness-of-fit criteria. The algorithm has been applied to a synthetic data set of partially clouded scenes and (non-cloud-screened) POLDER3/PARASOL observations.
S. J. Sutanto, G. Hoffmann, R. A. Scheepmaker, J. Worden, S. Houweling, K. Yoshimura, I. Aben, and T. Röckmann
Atmos. Meas. Tech., 8, 999–1019, https://doi.org/10.5194/amt-8-999-2015, https://doi.org/10.5194/amt-8-999-2015, 2015
D. J. Mrozek, C. van der Veen, M. Kliphuis, J. Kaiser, A. A. Wiegel, and T. Röckmann
Atmos. Meas. Tech., 8, 811–822, https://doi.org/10.5194/amt-8-811-2015, https://doi.org/10.5194/amt-8-811-2015, 2015
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Our analytical system is a promising tool for investigating the triple oxygen isotope composition of CO2 from stratospheric air samples of volumes 100ml and smaller. The method is designed for measuring air samples with CO2 mole fractions between 360 and 400ppm, and it is the first fully automated analytical system that uses CeO2 as the isotope exchange medium.
S. J. Sutanto, B. van den Hurk, P. A. Dirmeyer, S. I. Seneviratne, T. Röckmann, K. E. Trenberth, E. M. Blyth, J. Wenninger, and G. Hoffmann
Hydrol. Earth Syst. Sci., 18, 2815–2827, https://doi.org/10.5194/hess-18-2815-2014, https://doi.org/10.5194/hess-18-2815-2014, 2014
U. Dusek, M. Monaco, M. Prokopiou, F. Gongriep, R. Hitzenberger, H. A. J. Meijer, and T. Röckmann
Atmos. Meas. Tech., 7, 1943–1955, https://doi.org/10.5194/amt-7-1943-2014, https://doi.org/10.5194/amt-7-1943-2014, 2014
A. J. van Beelen, G. J. H. Roelofs, O. P. Hasekamp, J. S. Henzing, and T. Röckmann
Atmos. Chem. Phys., 14, 5969–5987, https://doi.org/10.5194/acp-14-5969-2014, https://doi.org/10.5194/acp-14-5969-2014, 2014
O. Peltola, A. Hensen, C. Helfter, L. Belelli Marchesini, F. C. Bosveld, W. C. M. van den Bulk, J. A. Elbers, S. Haapanala, J. Holst, T. Laurila, A. Lindroth, E. Nemitz, T. Röckmann, A. T. Vermeulen, and I. Mammarella
Biogeosciences, 11, 3163–3186, https://doi.org/10.5194/bg-11-3163-2014, https://doi.org/10.5194/bg-11-3163-2014, 2014
S. Houweling, M. Krol, P. Bergamaschi, C. Frankenberg, E. J. Dlugokencky, I. Morino, J. Notholt, V. Sherlock, D. Wunch, V. Beck, C. Gerbig, H. Chen, E. A. Kort, T. Röckmann, and I. Aben
Atmos. Chem. Phys., 14, 3991–4012, https://doi.org/10.5194/acp-14-3991-2014, https://doi.org/10.5194/acp-14-3991-2014, 2014
B. Ringeval, S. Houweling, P. M. van Bodegom, R. Spahni, R. van Beek, F. Joos, and T. Röckmann
Biogeosciences, 11, 1519–1558, https://doi.org/10.5194/bg-11-1519-2014, https://doi.org/10.5194/bg-11-1519-2014, 2014
M. E. Popa, M. K. Vollmer, A. Jordan, W. A. Brand, S. L. Pathirana, M. Rothe, and T. Röckmann
Atmos. Chem. Phys., 14, 2105–2123, https://doi.org/10.5194/acp-14-2105-2014, https://doi.org/10.5194/acp-14-2105-2014, 2014
D. Helmig, V. Petrenko, P. Martinerie, E. Witrant, T. Röckmann, A. Zuiderweg, R. Holzinger, J. Hueber, C. Thompson, J. W. C. White, W. Sturges, A. Baker, T. Blunier, D. Etheridge, M. Rubino, and P. Tans
Atmos. Chem. Phys., 14, 1463–1483, https://doi.org/10.5194/acp-14-1463-2014, https://doi.org/10.5194/acp-14-1463-2014, 2014
F. A. Haumann, A. M. Batenburg, G. Pieterse, C. Gerbig, M. C. Krol, and T. Röckmann
Atmos. Chem. Phys., 13, 9401–9413, https://doi.org/10.5194/acp-13-9401-2013, https://doi.org/10.5194/acp-13-9401-2013, 2013
M. von Hobe, S. Bekki, S. Borrmann, F. Cairo, F. D'Amato, G. Di Donfrancesco, A. Dörnbrack, A. Ebersoldt, M. Ebert, C. Emde, I. Engel, M. Ern, W. Frey, S. Genco, S. Griessbach, J.-U. Grooß, T. Gulde, G. Günther, E. Hösen, L. Hoffmann, V. Homonnai, C. R. Hoyle, I. S. A. Isaksen, D. R. Jackson, I. M. Jánosi, R. L. Jones, K. Kandler, C. Kalicinsky, A. Keil, S. M. Khaykin, F. Khosrawi, R. Kivi, J. Kuttippurath, J. C. Laube, F. Lefèvre, R. Lehmann, S. Ludmann, B. P. Luo, M. Marchand, J. Meyer, V. Mitev, S. Molleker, R. Müller, H. Oelhaf, F. Olschewski, Y. Orsolini, T. Peter, K. Pfeilsticker, C. Piesch, M. C. Pitts, L. R. Poole, F. D. Pope, F. Ravegnani, M. Rex, M. Riese, T. Röckmann, B. Rognerud, A. Roiger, C. Rolf, M. L. Santee, M. Scheibe, C. Schiller, H. Schlager, M. Siciliani de Cumis, N. Sitnikov, O. A. Søvde, R. Spang, N. Spelten, F. Stordal, O. Sumińska-Ebersoldt, A. Ulanovski, J. Ungermann, S. Viciani, C. M. Volk, M. vom Scheidt, P. von der Gathen, K. Walker, T. Wegner, R. Weigel, S. Weinbruch, G. Wetzel, F. G. Wienhold, I. Wohltmann, W. Woiwode, I. A. K. Young, V. Yushkov, B. Zobrist, and F. Stroh
Atmos. Chem. Phys., 13, 9233–9268, https://doi.org/10.5194/acp-13-9233-2013, https://doi.org/10.5194/acp-13-9233-2013, 2013
P. Sperlich, C. Buizert, T. M. Jenk, C. J. Sapart, M. Prokopiou, T. Röckmann, and T. Blunier
Atmos. Meas. Tech., 6, 2027–2041, https://doi.org/10.5194/amt-6-2027-2013, https://doi.org/10.5194/amt-6-2027-2013, 2013
J. Schmitt, B. Seth, M. Bock, C. van der Veen, L. Möller, C. J. Sapart, M. Prokopiou, T. Sowers, T. Röckmann, and H. Fischer
Atmos. Meas. Tech., 6, 1425–1445, https://doi.org/10.5194/amt-6-1425-2013, https://doi.org/10.5194/amt-6-1425-2013, 2013
S. Walter, A. Kock, and T. Röckmann
Biogeosciences, 10, 3391–3403, https://doi.org/10.5194/bg-10-3391-2013, https://doi.org/10.5194/bg-10-3391-2013, 2013
J. C. Laube, A. Keil, H. Bönisch, A. Engel, T. Röckmann, C. M. Volk, and W. T. Sturges
Atmos. Chem. Phys., 13, 2779–2791, https://doi.org/10.5194/acp-13-2779-2013, https://doi.org/10.5194/acp-13-2779-2013, 2013
N. Bândă, M. Krol, M. van Weele, T. van Noije, and T. Röckmann
Atmos. Chem. Phys., 13, 2267–2281, https://doi.org/10.5194/acp-13-2267-2013, https://doi.org/10.5194/acp-13-2267-2013, 2013
Sara M. Defratyka, Julianne M. Fernandez, Getachew A. Adnew, Guannan Dong, Peter M. J. Douglas, Daniel L. Eldridge, Giuseppe Etiope, Thomas Giunta, Mojhgan A. Haghnegahdar, Alexander N. Hristov, Nicole Hultquist, Iñaki Vadillo, Josue Jautzy, Ji-Hyun Kim, Jabrane Labidi, Ellen Lalk, Wil Leavitt, Jiawen Li, Li-Hung Lin, Jiarui Liu, Lucia Ojeda, Shuhei Ono, Jeemin Rhim, Thomas Röckmann, Barbara Sherwood Lollar, Malavika Sivan, Jiayang Sun, Gregory T. Ventura, David T. Wang, Edward D. Young, Naizhong Zhang, and Tim Arnold
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2025-41, https://doi.org/10.5194/essd-2025-41, 2025
Preprint under review for ESSD
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Measurement of methane’s doubly substituted isotopologues at natural abundances holds promise for better constraining the Earth’s atmospheric CH4 budget. We compiled 1475 measurements from field samples and laboratory experiments, conducted since 2014, to facilitate the differentiation of CH4 formation pathways and processes, to identify existing gaps limiting application of Δ13CH3D and Δ12CH2D2, and to develop isotope ratio source signature inputs for global CH4 flux modelling.
Eleftherios Ioannidis, Antoon Meesters, Michael Steiner, Dominik Brunner, Friedemann Reum, Isabelle Pison, Antoine Berchet, Rona Thompson, Espen Sollum, Frank-Thomas Koch, Christoph Gerbig, Fenjuan Wang, Shamil Maksyutov, Aki Tsuruta, Maria Tenkanen, Tuula Aalto, Guillaume Monteil, Hong Lin, Ge Ren, Marko Scholze, and Sander Houweling
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2025-235, https://doi.org/10.5194/essd-2025-235, 2025
Preprint under review for ESSD
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This paper describes a detailed study on CH4 European emissions, using different methodologies (9 total inverse models). The study spans over 15 years and provides detailed information on European CH4 emission trends and seasonality, using in-situ data, including ICOS network. Our results highlight the importance of improving details in the inversion setup, such as the treatment of lateral boundary conditions to narrow the uncertainty ranges further.
Bibhasvata Dasgupta, Malika Menoud, Carina van der Veen, Ingeborg Levin, Cora Veidt, Heiko Moossen, Sylvia Englund Michel, Peter Sperlich, Shinji Morimoto, Ryo Fujita, Taku Umezawa, Stephen Matthew Platt, Christine Groot Zwaaftink, Cathrine Lund Myhre, Rebecca Fisher, David Lowry, Euan Nisbet, James France, Ceres Woolley Maisch, Gordon Brailsford, Rowena Moss, Daisuke Goto, Sudhanshu Pandey, Sander Houweling, Nicola Warwick, and Thomas Röckmann
EGUsphere, https://doi.org/10.5194/egusphere-2025-2439, https://doi.org/10.5194/egusphere-2025-2439, 2025
This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
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We combined long-term methane mole fraction and isotope measurements from eight laboratories that sample high-latitude stations to compare, offset correct and harmonise the datasets into a hemisphere merged timeseries. Because each laboratory uses slightly different methods, we adjusted the data to make it directly comparable. This allowed us to create a consistent record of atmospheric methane concentration and its isotopes from 1988 to 2023.
Gerrit Kuhlmann, Foteini Stavropoulou, Stefan Schwietzke, Daniel Zavala-Araiza, Andrew Thorpe, Andreas Hueni, Lukas Emmenegger, Andreea Calcan, Thomas Röckmann, and Dominik Brunner
Atmos. Chem. Phys., 25, 5371–5385, https://doi.org/10.5194/acp-25-5371-2025, https://doi.org/10.5194/acp-25-5371-2025, 2025
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A measurement campaign in 2019 found that methane emissions from oil and gas in Romania were significantly higher than reported. In 2021, our follow-up campaign using airborne remote sensing showed a marked decreases in emissions by 20 %–60 % due to improved infrastructure. The study highlights the importance of measurement-based emission monitoring and illustrates the value of a multi-scale assessment integrating ground-based observations with large-scale airborne remote sensing campaigns.
Stavros Stagakis, Dominik Brunner, Junwei Li, Leif Backman, Anni Karvonen, Lionel Constantin, Leena Järvi, Minttu Havu, Jia Chen, Sophie Emberger, and Liisa Kulmala
Biogeosciences, 22, 2133–2161, https://doi.org/10.5194/bg-22-2133-2025, https://doi.org/10.5194/bg-22-2133-2025, 2025
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The balance between CO2 uptake and emissions from urban green areas is still not well understood. This study evaluated for the first time the urban park CO2 exchange simulations with four different types of biosphere model by comparing them with observations. Even though some advantages and disadvantages of the different model types were identified, there was no strong evidence that more complex models performed better than simple ones.
Simone Brunamonti, Harald Saathoff, Albert Hertzog, Glenn Diskin, Masatomo Fujiwara, Karen Rosenlof, Ottmar Möhler, Béla Tuzson, Lukas Emmenegger, Nadir Amarouche, Georges Durry, Fabien Frérot, Jean-Christophe Samake, Claire Cenac, Julio Lopez, Paul Monnier, and Mélanie Ghysels
EGUsphere, https://doi.org/10.5194/egusphere-2025-1029, https://doi.org/10.5194/egusphere-2025-1029, 2025
This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
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Water vapor is a strong greenhouse gas and accurate measurements of its concentration in the upper atmosphere (~8–25 km altitude) are crucial for reliable climate predictions. We investigated the performance of four airborne hygrometers, deployed on aircraft or stratospheric balloon platforms and based on different techniques, in a climate simulation chamber. The results demonstrate the high accuracy and reliability of the involved sensors for atmospheric monitoring and research applications.
Tanja J. Schuck, Johannes Degen, Timo Keber, Katharina Meixner, Thomas Wagenhäuser, Mélanie Ghysels, Georges Durry, Nadir Amarouche, Alessandro Zanchetta, Steven van Heuven, Huilin Chen, Johannes C. Laube, Sophie L. Baartman, Carina van der Veen, Maria Elena Popa, and Andreas Engel
Atmos. Chem. Phys., 25, 4333–4348, https://doi.org/10.5194/acp-25-4333-2025, https://doi.org/10.5194/acp-25-4333-2025, 2025
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A balloon was launched in 2021 in the Arctic to carry instruments for trace gas measurements up to 32 km. One purpose was to compare measurement techniques. We focus on the major greenhouse gases. To measure these, air was sampled with the AirCore technique and with flask sampling, and samples were analysed after the flight. In flight, observations were done with an optical method. In a companion paper, we report on observations of chlorine and bromine containing trace gases.
Dominik Brunner, Ivo Suter, Leonie Bernet, Lionel Constantin, Stuart K. Grange, Pascal Rubli, Junwei Li, Jia Chen, Alessandro Bigi, and Lukas Emmenegger
EGUsphere, https://doi.org/10.5194/egusphere-2025-640, https://doi.org/10.5194/egusphere-2025-640, 2025
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In order to support the city of Zurich in tracking its path to net-zero greenhouse gas emissions planned to be reached by 2040, a CO2 emission monitoring system was established. The system combines a dense network of CO2 sensors with a high-resolution atmospheric transport model GRAMM/GRAL. This study presents the setup of the model together with its numerous inputs and evaluates its performance in comparison with the observations from the CO2 sensor network.
Rainer Hilland, Josh Hashemi, Stavros Stagakis, Dominik Brunner, Lionel Constantin, Natascha Kljun, Betty Molinier, Samuel Hammer, Lukas Emmenegger, and Andreas Christen
EGUsphere, https://doi.org/10.5194/egusphere-2025-1088, https://doi.org/10.5194/egusphere-2025-1088, 2025
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We present a study of simultaneously measured fluxes of carbon dioxide (CO2) and co-emitted species in the city of Zurich. Flux measurements of CO2 alone can’t be attributed to specific emission sectors, such as road transport or residential heating. We present a model which uses the measured ratios of CO2 to carbon monoxide (CO) and nitrogen oxides (NOx) as well as sector-specific reference ratios, to attribute measured fluxes to their emission sectors.
Eric Förster, Heidi Huntrieser, Michael Lichtenstern, Falk Pätzold, Lutz Bretschneider, Andreas Schlerf, Sven Bollmann, Astrid Lampert, Jarosław Nęcki, Paweł Jagoda, Justyna Swolkień, Dominika Pasternak, Robert A. Field, and Anke Roiger
EGUsphere, https://doi.org/10.5194/egusphere-2025-1010, https://doi.org/10.5194/egusphere-2025-1010, 2025
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We introduce a helicopter-borne mass balance approach, utilizing the HELiPOD platform, to accurately quantify methane (CH₄) emissions from coal mining activities. The comparison of our top-down mass flux estimates (up to 3000 kg h-1) against those from bottom-up in-mine CH4 safety sensors revealed very good agreement. This approach also has a great potential in quantifying emission source strengths (down to 20 kg h-1) from a wide range of other CH4 emitters (e.g. landfills, oil & gas industry).
Joël Thanwerdas, Antoine Berchet, Lionel Constantin, Aki Tsuruta, Michael Steiner, Friedemann Reum, Stephan Henne, and Dominik Brunner
Geosci. Model Dev., 18, 1505–1544, https://doi.org/10.5194/gmd-18-1505-2025, https://doi.org/10.5194/gmd-18-1505-2025, 2025
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The Community Inversion Framework (CIF) brings together methods for estimating greenhouse gas fluxes from atmospheric observations. The initial ensemble method implemented in CIF was found to be incomplete and could hardly be compared to other ensemble methods employed in the inversion community. In this paper, we present and evaluate a new implementation of the ensemble mode, building upon the initial developments.
Robbert Petrus Johannes Moonen, Getachew Agmuas Adnew, Jordi Vilà-Guerau de Arellano, Oscar Karel Hartogensis, David Joan Bonell Fontas, Shujiro Komiya, Sam P. Jones, and Thomas Röckmann
EGUsphere, https://doi.org/10.5194/egusphere-2025-452, https://doi.org/10.5194/egusphere-2025-452, 2025
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Understory ejections are distinct turbulent features emerging in prime tall forest ecosystems. We share a method to isolate understory ejections based on H2O-CO2 anomalie quadrants. From these, we calculate the flux contributions of understory ejections and all flux quadrants. In addition we show that a distinctly depleted isotopic composition can be found in the ejected water vapour. Finally, we explored the role of clouds as a potential trigger for understory ejections.
Stuart K. Grange, Pascal Rubli, Andrea Fischer, Dominik Brunner, Christoph Hueglin, and Lukas Emmenegger
Atmos. Chem. Phys., 25, 2781–2806, https://doi.org/10.5194/acp-25-2781-2025, https://doi.org/10.5194/acp-25-2781-2025, 2025
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Carbon dioxide (CO2) is a very important atmospheric pollutant, and to better understand the gas's source and sink dynamics, a mid-cost sensor network hosting 26 sites was deployed in and around Zurich, Switzerland. The sensor measurement performance was quantified, and natural and anthropogenic CO2 emission sources were explored with a focus on what drives high CO2 levels. The observations will be used further by others to validate what is thought to be known about CO2 emissions in the region.
Hector Navarro-Barboza, Jordi Rovira, Vincenzo Obiso, Andrea Pozzer, Marta Via, Andres Alastuey, Xavier Querol, Noemi Perez, Marjan Savadkoohi, Gang Chen, Jesus Yus-Díez, Matic Ivancic, Martin Rigler, Konstantinos Eleftheriadis, Stergios Vratolis, Olga Zografou, Maria Gini, Benjamin Chazeau, Nicolas Marchand, Andre S. H. Prevot, Kaspar Dallenbach, Mikael Ehn, Krista Luoma, Tuukka Petäjä, Anna Tobler, Jaroslaw Necki, Minna Aurela, Hilkka Timonen, Jarkko Niemi, Olivier Favez, Jean-Eudes Petit, Jean-Philippe Putaud, Christoph Hueglin, Nicolas Pascal, Aurélien Chauvigné, Sébastien Conil, Marco Pandolfi, and Oriol Jorba
Atmos. Chem. Phys., 25, 2667–2694, https://doi.org/10.5194/acp-25-2667-2025, https://doi.org/10.5194/acp-25-2667-2025, 2025
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Brown carbon (BrC) absorbs ultraviolet (UV) and visible light, influencing climate. This study explores BrC's imaginary refractive index (k) using data from 12 European sites. Residential emissions are a major organic aerosol (OA) source in winter, while secondary organic aerosol (SOA) dominates in summer. Source-specific k values were derived, improving model accuracy. The findings highlight BrC's climate impact and emphasize source-specific constraints in atmospheric models.
Hossein Maazallahi, Foteini Stavropoulou, Samuel Jonson Sutanto, Michael Steiner, Dominik Brunner, Mariano Mertens, Patrick Jöckel, Antoon Visschedijk, Hugo Denier van der Gon, Stijn Dellaert, Nataly Velandia Salinas, Stefan Schwietzke, Daniel Zavala-Araiza, Sorin Ghemulet, Alexandru Pana, Magdalena Ardelean, Marius Corbu, Andreea Calcan, Stephen A. Conley, Mackenzie L. Smith, and Thomas Röckmann
Atmos. Chem. Phys., 25, 1497–1511, https://doi.org/10.5194/acp-25-1497-2025, https://doi.org/10.5194/acp-25-1497-2025, 2025
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This article presents insights from airborne in situ measurements collected during the ROmanian Methane Emissions from Oil and gas (ROMEO) campaign supported by two models. Results reveal Romania's oil and gas methane emissions were significantly under-reported to the United Nations Framework Convention on Climate Change (UNFCCC) in 2019. A large underestimation was also found in the Emissions Database for Global Atmospheric Research (EDGAR) v7.0 for the study domain in the same year.
Sophie L. Baartman, Steven M. Driever, Maarten Wassenaar, Linda M. J. Kooijmans, Nerea Ubierna Lopez, Leon Mossink, Maria E. Popa, Ara Cho, Lisa Wingate, Thomas Röckmann, Steven M. A. C. van Heuven, and Maarten C. Krol
EGUsphere, https://doi.org/10.5194/egusphere-2025-215, https://doi.org/10.5194/egusphere-2025-215, 2025
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Carbonyl sulfide (COS) and carbon dioxide (CO2) uptake fluxes and isotope discrimination was measured in sunflower and papyrus plants, using a plant chamber approach and varying light availability. COS and CO2 isotope discrimination in plants have never been jointly measured before. COS isotope discrimination did not differ between the species, nor with changing light. CO2 fluxes and isotope values provided additional useful information for data interpretation.
Pieter Rijsdijk, Henk Eskes, Arlene Dingemans, K. Folkert Boersma, Takashi Sekiya, Kazuyuki Miyazaki, and Sander Houweling
Geosci. Model Dev., 18, 483–509, https://doi.org/10.5194/gmd-18-483-2025, https://doi.org/10.5194/gmd-18-483-2025, 2025
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Clustering high-resolution satellite observations into superobservations improves model validation and data assimilation applications. In our paper, we derive quantitative uncertainties for satellite NO2 column observations based on knowledge of the retrievals, including a detailed analysis of spatial error correlations and representativity errors. The superobservations and uncertainty estimates are tested in a global chemical data assimilation system and are found to improve the forecasts.
Judith Tettenborn, Daniel Zavala-Araiza, Daan Stroeken, Hossein Maazallahi, Carina van der Veen, Arjan Hensen, Ilona Velzeboer, Pim van den Bulk, Felix Vogel, Lawson Gillespie, Sebastien Ars, James France, David Lowry, Rebecca Fisher, and Thomas Röckmann
EGUsphere, https://doi.org/10.5194/egusphere-2024-3620, https://doi.org/10.5194/egusphere-2024-3620, 2025
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Measurements of methane with vehicle-based sensors are an effective method to identify and quantify leaks from urban gas distribution systems. We deliberately released methane in different environments, and calibrated the response of different methane analyzers when they transect the plumes in a vehicle. We derived an improved statistical function for consistent emission estimations using different instruments. Repeated transects reduce the uncertainty in emission rate estimates.
Diego Santaren, Janne Hakkarainen, Gerrit Kuhlmann, Erik Koene, Frédéric Chevallier, Iolanda Ialongo, Hannakaisa Lindqvist, Janne Nurmela, Johanna Tamminen, Laia Amorós, Dominik Brunner, and Grégoire Broquet
Atmos. Meas. Tech., 18, 211–239, https://doi.org/10.5194/amt-18-211-2025, https://doi.org/10.5194/amt-18-211-2025, 2025
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This study evaluates data-driven inversion methods for estimating CO2 emissions from local sources, such as power plants and cities, using meteorological data and XCO2 and NO2 satellite images rather than atmospheric transport modeling. We assess and compare the performance of five different methods using simulations of 1 year of satellite images, taken from the upcoming Copernicus CO2 Monitoring Mission, covering 15 power plants and the city of Berlin, Germany.
Carlos Gómez-Ortiz, Guillaume Monteil, Sourish Basu, and Marko Scholze
Atmos. Chem. Phys., 25, 397–424, https://doi.org/10.5194/acp-25-397-2025, https://doi.org/10.5194/acp-25-397-2025, 2025
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In this paper, we test new implementations of our inverse modeling tool to estimate the weekly and regional CO2 emissions from fossil fuels in Europe. We use synthetic atmospheric observations of CO2 and radiocarbon (14CO2) to trace emissions to their sources, while separating the natural and fossil CO2. Our tool accurately estimates fossil CO2 emissions in densely monitored regions like western/central Europe. This approach aids in developing strategies for reducing CO2 emissions.
Johannes C. Laube, Tanja J. Schuck, Huilin Chen, Markus Geldenhuys, Steven van Heuven, Timo Keber, Maria Elena Popa, Elinor Tuffnell, Bärbel Vogel, Thomas Wagenhäuser, Alessandro Zanchetta, and Andreas Engel
EGUsphere, https://doi.org/10.5194/egusphere-2024-4034, https://doi.org/10.5194/egusphere-2024-4034, 2025
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A large balloon was launched in summer 2021 in the Arctic to carry instruments for trace gas measurements up to 32 km, above the reach of aircraft. The main aims were to evaluate different techniques and atmospheric processes. We focus on halogenated greenhouse gases and ozone-depleting substances. For this, air was collected with the AirCore technique and a cryogenic air sampler and measured after the flight. A companion paper reports observations of major greenhouse gases.
Carlos Gómez-Ortiz, Guillaume Monteil, Ute Karstens, and Marko Scholze
EGUsphere, https://doi.org/10.5194/egusphere-2024-3013, https://doi.org/10.5194/egusphere-2024-3013, 2025
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In 2024, an intensive sampling campaign is being conducted to improve fossil CO₂ emission estimates in Europe using 14C measurements. By testing different strategies for selecting air samples, this study shows that increasing sample frequency and carefully choosing samples based on their fossil fuel and nuclear content leads to more accurate results, reducing the uncertainty and bias of the estimates.
Guillaume Monteil, Jalisha Theanutti Kallingal, and Marko Scholze
EGUsphere, https://doi.org/10.5194/egusphere-2024-3122, https://doi.org/10.5194/egusphere-2024-3122, 2024
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Methane is a potent greenhouse gas, emitted both from natural and anthropogenic processes. Large uncertainties remain on its emission budget. Our study compares and combines two approaches to estimate European methane emissions, with a focus on wetlands, based on observed atmospheric CH4 concentrations and in-situ flux measurements. We find a good agreement and complementarity between the approaches, and identify obstacles towards a more integrated data-informed emission estimation system.
Yuri Brugnara, Martin Steinbacher, Simone Baffelli, and Lukas Emmenegger
EGUsphere, https://doi.org/10.5194/egusphere-2024-3556, https://doi.org/10.5194/egusphere-2024-3556, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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GAW-QC is an interactive dashboard for the quality control of in-situ atmospheric composition measurements made at stations taking part in the Global Atmosphere Watch network. Even though it is mainly targeted at station operators who want to analyze recent, not yet published measurements, it allows anybody to verify the quality of already published measurements using various anomaly detection algorithms as well as visual comparisons.
Arseniy Karagodin-Doyennel, Fredrik Jansson, Bart van Stratum, Hugo Denier van der Gon, Jordi Vilà-Guerau de Arellano, and Sander Houweling
EGUsphere, https://doi.org/10.5194/egusphere-2024-3721, https://doi.org/10.5194/egusphere-2024-3721, 2024
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We introduce a new simulation platform based on the Dutch Large-Eddy Simulation (DALES) to simulate carbon dioxide (CO2) emissions and their dispersion in the turbulent environments with hectometer resolution. This model incorporates both anthropogenic emission inventory and ecosystem exchanges. Simulation results for the main urban area in the Netherlands demonstrate a strong potential of DALES to enhance CO2 emission modeling, which is important for refining their reduction strategies.
Jakob Pernov, William Aeberhard, Michele Volpi, Eliza Harris, Benjamin Hohermuth, Sakiko Ishino, Ragnhild Bieltvedt Skeie, Stephan Henne, Ulas Im, Patricia Quinn, Lucia Upchurch, and Julia Schmale
EGUsphere, https://doi.org/10.5194/egusphere-2024-3379, https://doi.org/10.5194/egusphere-2024-3379, 2024
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MSAp is a vital part of the Arctic climate system. Numerical models struggle to reproduce the seasonal cycle of MSAp. We evaluate three numerical models and one reanalysis product’s ability to simulate MSAp. We develop data-driven models for MSAp at four High Arctic stations. The data-driven models outperform the numerical models and reanalysis product and identified precursor source, chemical processing, and removal-related features as being important for modeling MSAp.
Getachew Agmuas Adnew, Gerbrand Koren, Neha Mehendale, Sergey Gromov, Maarten Krol, and Thomas Röckmann
EGUsphere, https://doi.org/10.5194/egusphere-2024-3231, https://doi.org/10.5194/egusphere-2024-3231, 2024
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This study presents high-precision measurements of ∆′17O(CO2). Key findings include the extension of the N2O-∆′17O correlation to the upper troposphere and the identification of significant differences in the N2O-∆′17O slope in StratoClim samples. Additionally, the ∆′17O measurements are used to estimate global stratospheric production and surface removal of ∆′17O, providing an independent estimate of global vegetation CO2 exchange.
Michael Steiner, Luca Cantarello, Stephan Henne, and Dominik Brunner
Atmos. Chem. Phys., 24, 12447–12463, https://doi.org/10.5194/acp-24-12447-2024, https://doi.org/10.5194/acp-24-12447-2024, 2024
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Atmospheric greenhouse gas inversions have great potential to independently check reported bottom-up emissions; however they are subject to large uncertainties. It is paramount to address and reduce the largest source of uncertainty, which stems from the representation of atmospheric transport in the models. In this study, we show that the use of a temporally varying flow-dependent atmospheric transport uncertainty can enhance the accuracy of emission estimation in an idealized experiment.
Ana Maria Roxana Petrescu, Glen P. Peters, Richard Engelen, Sander Houweling, Dominik Brunner, Aki Tsuruta, Bradley Matthews, Prabir K. Patra, Dmitry Belikov, Rona L. Thompson, Lena Höglund-Isaksson, Wenxin Zhang, Arjo J. Segers, Giuseppe Etiope, Giancarlo Ciotoli, Philippe Peylin, Frédéric Chevallier, Tuula Aalto, Robbie M. Andrew, David Bastviken, Antoine Berchet, Grégoire Broquet, Giulia Conchedda, Stijn N. C. Dellaert, Hugo Denier van der Gon, Johannes Gütschow, Jean-Matthieu Haussaire, Ronny Lauerwald, Tiina Markkanen, Jacob C. A. van Peet, Isabelle Pison, Pierre Regnier, Espen Solum, Marko Scholze, Maria Tenkanen, Francesco N. Tubiello, Guido R. van der Werf, and John R. Worden
Earth Syst. Sci. Data, 16, 4325–4350, https://doi.org/10.5194/essd-16-4325-2024, https://doi.org/10.5194/essd-16-4325-2024, 2024
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This study provides an overview of data availability from observation- and inventory-based CH4 emission estimates. It systematically compares them and provides recommendations for robust comparisons, aiming to steadily engage more parties in using observational methods to complement their UNFCCC submissions. Anticipating improvements in atmospheric modelling and observations, future developments need to resolve knowledge gaps in both approaches and to better quantify remaining uncertainty.
Yosuke Niwa, Yasunori Tohjima, Yukio Terao, Tazu Saeki, Akihiko Ito, Taku Umezawa, Kyohei Yamada, Motoki Sasakawa, Toshinobu Machida, Shin-Ichiro Nakaoka, Hideki Nara, Hiroshi Tanimoto, Hitoshi Mukai, Yukio Yoshida, Shinji Morimoto, Shinya Takatsuji, Kazuhiro Tsuboi, Yousuke Sawa, Hidekazu Matsueda, Kentaro Ishijima, Ryo Fujita, Daisuke Goto, Xin Lan, Kenneth Schuldt, Michal Heliasz, Tobias Biermann, Lukasz Chmura, Jarsolaw Necki, and Irène Xueref-Remy
EGUsphere, https://doi.org/10.5194/egusphere-2024-2457, https://doi.org/10.5194/egusphere-2024-2457, 2024
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This study estimated regional and sectoral emission contributions to the unprecedented surge of atmospheric methane for 2020–2022. The methane is the second most important greenhouse gas and its emissions reduction is urgently required to mitigate the global warming. Numerical modeling-based estimates with three different sets of atmospheric observations consistently suggested large contributions of biogenic emissions from South Asia and Southeast Asia to the surge of atmospheric methane.
Eliza Harris, Philipp Fischer, Maciej P. Lewicki, Dominika Lewicka-Szczebak, Stephen J. Harris, and Fernando Perez-Cruz
Biogeosciences, 21, 3641–3663, https://doi.org/10.5194/bg-21-3641-2024, https://doi.org/10.5194/bg-21-3641-2024, 2024
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Greenhouse gases are produced and consumed via a number of pathways. Quantifying these pathways helps reduce the climate and environmental footprint of anthropogenic activities. The contribution of the pathways can be estimated from the isotopic composition, which acts as a fingerprint for these pathways. We have developed the Time-resolved FRactionation And Mixing Evaluation (TimeFRAME) model to simplify interpretation and estimate the contribution of different pathways and their uncertainty.
Hella van Asperen, Thorsten Warneke, Alessandro Carioca de Araújo, Bruce Forsberg, Sávio José Filgueiras Ferreira, Thomas Röckmann, Carina van der Veen, Sipko Bulthuis, Leonardo Ramos de Oliveira, Thiago de Lima Xavier, Jailson da Mata, Marta de Oliveira Sá, Paulo Ricardo Teixeira, Julie Andrews de França e Silva, Susan Trumbore, and Justus Notholt
Biogeosciences, 21, 3183–3199, https://doi.org/10.5194/bg-21-3183-2024, https://doi.org/10.5194/bg-21-3183-2024, 2024
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Carbon monoxide (CO) is regarded as an important indirect greenhouse gas. Soils can emit and take up CO, but, until now, uncertainty remains as to which process dominates in tropical rainforests. We present the first soil CO flux measurements from a tropical rainforest. Based on our observations, we report that tropical rainforest soils are a net source of CO. In addition, we show that valley streams and inundated areas are likely additional hot spots of CO in the ecosystem.
Sandro Meier, Erik F. M. Koene, Maarten Krol, Dominik Brunner, Alexander Damm, and Gerrit Kuhlmann
Atmos. Chem. Phys., 24, 7667–7686, https://doi.org/10.5194/acp-24-7667-2024, https://doi.org/10.5194/acp-24-7667-2024, 2024
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Nitrogen oxides (NOx = NO + NO2) are important air pollutants. This study addresses the challenge of accurately estimating NOx emissions from NO2 satellite observations. We develop a realistic model to convert NO2 to NOx by using simulated plumes from various power plants. We apply the model to satellite NO2 observations, significantly reducing biases in estimated NOx emissions. The study highlights the potential for a consistent, high-resolution estimation of NOx emissions using satellite data.
Gerrit Kuhlmann, Erik Koene, Sandro Meier, Diego Santaren, Grégoire Broquet, Frédéric Chevallier, Janne Hakkarainen, Janne Nurmela, Laia Amorós, Johanna Tamminen, and Dominik Brunner
Geosci. Model Dev., 17, 4773–4789, https://doi.org/10.5194/gmd-17-4773-2024, https://doi.org/10.5194/gmd-17-4773-2024, 2024
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We present a Python software library for data-driven emission quantification (ddeq). It can be used to determine the emissions of hot spots (cities, power plants and industry) from remote sensing images using different methods. ddeq can be extended for new datasets and methods, providing a powerful community tool for users and developers. The application of the methods is shown using Jupyter notebooks included in the library.
Jin Ma, Linda M. J. Kooijmans, Norbert Glatthor, Stephen A. Montzka, Marc von Hobe, Thomas Röckmann, and Maarten C. Krol
Atmos. Chem. Phys., 24, 6047–6070, https://doi.org/10.5194/acp-24-6047-2024, https://doi.org/10.5194/acp-24-6047-2024, 2024
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The global budget of atmospheric COS can be optimised by inverse modelling using TM5-4DVAR, with the co-constraints of NOAA surface observations and MIPAS satellite data. We found reduced COS biosphere uptake from inversions and improved land and ocean separation using MIPAS satellite data assimilation. Further improvements are expected from better quantification of COS ocean and biosphere fluxes.
Katrine A. Gorham, Sam Abernethy, Tyler R. Jones, Peter Hess, Natalie M. Mahowald, Daphne Meidan, Matthew S. Johnson, Maarten M. J. W. van Herpen, Yangyang Xu, Alfonso Saiz-Lopez, Thomas Röckmann, Chloe A. Brashear, Erika Reinhardt, and David Mann
Atmos. Chem. Phys., 24, 5659–5670, https://doi.org/10.5194/acp-24-5659-2024, https://doi.org/10.5194/acp-24-5659-2024, 2024
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Rapid reduction in atmospheric methane is needed to slow the rate of global warming. Reducing anthropogenic methane emissions is a top priority. However, atmospheric methane is also impacted by rising natural emissions and changing sinks. Studies of possible atmospheric methane removal approaches, such as iron salt aerosols to increase the chlorine radical sink, benefit from a roadmapped approach to understand if there may be viable and socially acceptable ways to decrease future risk.
Malavika Sivan, Thomas Röckmann, Carina van der Veen, and Maria Elena Popa
Atmos. Meas. Tech., 17, 2687–2705, https://doi.org/10.5194/amt-17-2687-2024, https://doi.org/10.5194/amt-17-2687-2024, 2024
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We have set up a measurement system for methane-clumped isotopologues. We have built an extraction and purification system to extract pure methane for these measurements, for samples of various origins, including atmospheric air, for which we need to process about 1000 L of air for one measurement. We report here the technical setup for extraction and measurements, as well as the calibration, and we give an overview of the samples measured so far.
Mirosław Zimnoch, Michał Gałkowski, Piotr Sekuła, Łukasz Chmura, Jakub Bartyzel, Alina Jasek-Kamińska, Alicja Skiba, Jarosław Nęcki, Przemysław Wachniew, and Paweł Jagoda
EGUsphere, https://doi.org/10.5194/egusphere-2024-1167, https://doi.org/10.5194/egusphere-2024-1167, 2024
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The manuscript presents the dataset collected in the urban area of Krakow city containing several measurement campaigns focused on the investigation of vertical CO2 and CH4 profiles supplemented by set of meteorological parameters (e.g. temperature, pressure) measured along the profiles up to ca. 280 m a.g.l. The presented data collection explains the dynamics of the lower atmosphere on a daily and seasonal scale providing the three dimensional dataset that can be used for model validation.
Susanne Preunkert, Pascal Bohleber, Michel Legrand, Adrien Gilbert, Tobias Erhardt, Roland Purtschert, Lars Zipf, Astrid Waldner, Joseph R. McConnell, and Hubertus Fischer
The Cryosphere, 18, 2177–2194, https://doi.org/10.5194/tc-18-2177-2024, https://doi.org/10.5194/tc-18-2177-2024, 2024
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Ice cores from high-elevation Alpine glaciers are an important tool to reconstruct the past atmosphere. However, since crevasses are common at these glacier sites, rigorous investigations of glaciological conditions upstream of drill sites are needed before interpreting such ice cores. On the basis of three ice cores extracted at Col du Dôme (4250 m a.s.l; French Alps), an overall picture of a dynamic crevasse formation is drawn, which disturbs the depth–age relation of two of the three cores.
Emily Dowd, Alistair J. Manning, Bryn Orth-Lashley, Marianne Girard, James France, Rebecca E. Fisher, Dave Lowry, Mathias Lanoisellé, Joseph R. Pitt, Kieran M. Stanley, Simon O'Doherty, Dickon Young, Glen Thistlethwaite, Martyn P. Chipperfield, Emanuel Gloor, and Chris Wilson
Atmos. Meas. Tech., 17, 1599–1615, https://doi.org/10.5194/amt-17-1599-2024, https://doi.org/10.5194/amt-17-1599-2024, 2024
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We provide the first validation of the satellite-derived emission estimates using surface-based mobile greenhouse gas surveys of an active gas leak detected near Cheltenham, UK. GHGSat’s emission estimates broadly agree with the surface-based mobile survey and steps were taken to fix the leak, highlighting the importance of satellite data in identifying emissions and helping to reduce our human impact on climate change.
Michael Steiner, Wouter Peters, Ingrid Luijkx, Stephan Henne, Huilin Chen, Samuel Hammer, and Dominik Brunner
Atmos. Chem. Phys., 24, 2759–2782, https://doi.org/10.5194/acp-24-2759-2024, https://doi.org/10.5194/acp-24-2759-2024, 2024
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The Paris Agreement increased interest in estimating greenhouse gas (GHG) emissions of individual countries, but top-down emission estimation is not yet considered policy-relevant. It is therefore paramount to reduce large errors and to build systems that are based on the newest atmospheric transport models. In this study, we present the first application of ICON-ART in the inverse modeling of GHG fluxes with an ensemble Kalman filter and present our results for European CH4 emissions.
Robert Hanfland, Dominik Brunner, Christiane Voigt, Alina Fiehn, Anke Roiger, and Margit Pattantyús-Ábrahám
Atmos. Chem. Phys., 24, 2511–2534, https://doi.org/10.5194/acp-24-2511-2024, https://doi.org/10.5194/acp-24-2511-2024, 2024
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To show that the three-dimensional dispersion of plumes simulated by the Atmospheric Radionuclide Transport Model within the planetary boundary layer agrees with real plumes, we identify the most important input parameters and analyse the turbulence properties of five different turbulence models in very unstable stratification conditions using their deviation from the well-mixed state. Simulations show that one model agrees slightly better in unstable stratification conditions.
Magdalena Pühl, Anke Roiger, Alina Fiehn, Alan M. Gorchov Negron, Eric A. Kort, Stefan Schwietzke, Ignacio Pisso, Amy Foulds, James Lee, James L. France, Anna E. Jones, Dave Lowry, Rebecca E. Fisher, Langwen Huang, Jacob Shaw, Prudence Bateson, Stephen Andrews, Stuart Young, Pamela Dominutti, Tom Lachlan-Cope, Alexandra Weiss, and Grant Allen
Atmos. Chem. Phys., 24, 1005–1024, https://doi.org/10.5194/acp-24-1005-2024, https://doi.org/10.5194/acp-24-1005-2024, 2024
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In April–May 2019 we carried out an airborne field campaign in the southern North Sea with the aim of studying methane emissions of offshore gas installations. We determined methane emissions from elevated methane measured downstream of the sampled installations. We compare our measured methane emissions with estimated methane emissions from national and global annual inventories. As a result, we find inconsistencies of inventories and large discrepancies between measurements and inventories.
Alina Fiehn, Maximilian Eckl, Julian Kostinek, Michał Gałkowski, Christoph Gerbig, Michael Rothe, Thomas Röckmann, Malika Menoud, Hossein Maazallahi, Martina Schmidt, Piotr Korbeń, Jarosław Neçki, Mila Stanisavljević, Justyna Swolkień, Andreas Fix, and Anke Roiger
Atmos. Chem. Phys., 23, 15749–15765, https://doi.org/10.5194/acp-23-15749-2023, https://doi.org/10.5194/acp-23-15749-2023, 2023
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During the CoMet mission in the Upper Silesian Coal Basin (USCB) ground-based and airborne air samples were taken and analyzed for the isotopic composition of CH4 to derive the mean signature of the USCB and source signatures of individual coal mines. Using δ2H signatures, the biogenic emissions from the USCB account for 15 %–50 % of total emissions, which is underestimated in common emission inventories. This demonstrates the importance of δ2H-CH4 observations for methane source apportionment.
Robbert P. J. Moonen, Getachew A. Adnew, Oscar K. Hartogensis, Jordi Vilà-Guerau de Arellano, David J. Bonell Fontas, and Thomas Röckmann
Atmos. Meas. Tech., 16, 5787–5810, https://doi.org/10.5194/amt-16-5787-2023, https://doi.org/10.5194/amt-16-5787-2023, 2023
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Isotope fluxes allow for net ecosystem gas exchange fluxes to be partitioned into sub-components like plant assimilation, respiration and transpiration, which can help us better understand the environmental drivers of each partial flux. We share the results of a field campaign isotope fluxes were derived using a combination of laser spectroscopy and eddy covariance. We found lag times and high frequency signal loss in the isotope fluxes we derived and present methods to correct for both.
Leonard Kirago, Örjan Gustafsson, Samuel Mwaniki Gaita, Sophie L. Haslett, Michael J. Gatari, Maria Elena Popa, Thomas Röckmann, Christoph Zellweger, Martin Steinbacher, Jörg Klausen, Christian Félix, David Njiru, and August Andersson
Atmos. Chem. Phys., 23, 14349–14357, https://doi.org/10.5194/acp-23-14349-2023, https://doi.org/10.5194/acp-23-14349-2023, 2023
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This study provides ground-observational evidence that supports earlier suggestions that savanna fires are the main emitters and modulators of carbon monoxide gas in Africa. Using isotope-based techniques, the study has shown that about two-thirds of this gas is emitted from savanna fires, while for urban areas, in this case Nairobi, primary sources approach 100 %. The latter has implications for air quality policy, suggesting primary emissions such as traffic should be targeted.
Tobias Erhardt, Camilla Marie Jensen, Florian Adolphi, Helle Astrid Kjær, Remi Dallmayr, Birthe Twarloh, Melanie Behrens, Motohiro Hirabayashi, Kaori Fukuda, Jun Ogata, François Burgay, Federico Scoto, Ilaria Crotti, Azzurra Spagnesi, Niccoló Maffezzoli, Delia Segato, Chiara Paleari, Florian Mekhaldi, Raimund Muscheler, Sophie Darfeuil, and Hubertus Fischer
Earth Syst. Sci. Data, 15, 5079–5091, https://doi.org/10.5194/essd-15-5079-2023, https://doi.org/10.5194/essd-15-5079-2023, 2023
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The presented paper provides a 3.8 kyr long dataset of aerosol concentrations from the East Greenland Ice coring Project (EGRIP) ice core. The data consists of 1 mm depth-resolution profiles of calcium, sodium, ammonium, nitrate, and electrolytic conductivity as well as decadal averages of these profiles. Alongside the data a detailed description of the measurement setup as well as a discussion of the uncertainties are given.
Ioannis Katharopoulos, Dominique Rust, Martin K. Vollmer, Dominik Brunner, Stefan Reimann, Simon J. O'Doherty, Dickon Young, Kieran M. Stanley, Tanja Schuck, Jgor Arduini, Lukas Emmenegger, and Stephan Henne
Atmos. Chem. Phys., 23, 14159–14186, https://doi.org/10.5194/acp-23-14159-2023, https://doi.org/10.5194/acp-23-14159-2023, 2023
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The effectiveness of climate change mitigation needs to be scrutinized by monitoring greenhouse gas (GHG) emissions. Countries report their emissions to the UN in a bottom-up manner. By combining atmospheric observations and transport models someone can independently validate emission estimates in a top-down fashion. We report Swiss emissions of synthetic GHGs based on kilometer-scale transport and inverse modeling, highlighting the role of appropriate resolution in complex terrain.
Hossein Maazallahi, Antonio Delre, Charlotte Scheutz, Anders M. Fredenslund, Stefan Schwietzke, Hugo Denier van der Gon, and Thomas Röckmann
Atmos. Meas. Tech., 16, 5051–5073, https://doi.org/10.5194/amt-16-5051-2023, https://doi.org/10.5194/amt-16-5051-2023, 2023
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Measurement methods are increasingly deployed to verify reported methane emissions of gas leaks. This study describes unique advantages and limitations of three methods. Two methods are rapidly deployed, but uncertainties and biases exist for some leak locations. In contrast, the suction method could accurately determine leak rates in principle. However, this method, which provides data for the German emission inventory, creates an overall low bias in our study due to non-random site selection.
Simone Brunamonti, Manuel Graf, Tobias Bühlmann, Céline Pascale, Ivan Ilak, Lukas Emmenegger, and Béla Tuzson
Atmos. Meas. Tech., 16, 4391–4407, https://doi.org/10.5194/amt-16-4391-2023, https://doi.org/10.5194/amt-16-4391-2023, 2023
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The abundance of water vapor (H2O) in the upper atmosphere has a significant impact on the rate of global warming. We developed a new lightweight spectrometer (ALBATROSS) for H2O measurements aboard meteorological balloons. Here, we assess the accuracy and precision of ALBATROSS using metrology-grade reference gases. The results demonstrate the exceptional potential of mid-infrared laser absorption spectroscopy as a new reference method for in situ measurements of H2O in the upper atmosphere.
Matthew J. McGrath, Ana Maria Roxana Petrescu, Philippe Peylin, Robbie M. Andrew, Bradley Matthews, Frank Dentener, Juraj Balkovič, Vladislav Bastrikov, Meike Becker, Gregoire Broquet, Philippe Ciais, Audrey Fortems-Cheiney, Raphael Ganzenmüller, Giacomo Grassi, Ian Harris, Matthew Jones, Jürgen Knauer, Matthias Kuhnert, Guillaume Monteil, Saqr Munassar, Paul I. Palmer, Glen P. Peters, Chunjing Qiu, Mart-Jan Schelhaas, Oksana Tarasova, Matteo Vizzarri, Karina Winkler, Gianpaolo Balsamo, Antoine Berchet, Peter Briggs, Patrick Brockmann, Frédéric Chevallier, Giulia Conchedda, Monica Crippa, Stijn N. C. Dellaert, Hugo A. C. Denier van der Gon, Sara Filipek, Pierre Friedlingstein, Richard Fuchs, Michael Gauss, Christoph Gerbig, Diego Guizzardi, Dirk Günther, Richard A. Houghton, Greet Janssens-Maenhout, Ronny Lauerwald, Bas Lerink, Ingrid T. Luijkx, Géraud Moulas, Marilena Muntean, Gert-Jan Nabuurs, Aurélie Paquirissamy, Lucia Perugini, Wouter Peters, Roberto Pilli, Julia Pongratz, Pierre Regnier, Marko Scholze, Yusuf Serengil, Pete Smith, Efisio Solazzo, Rona L. Thompson, Francesco N. Tubiello, Timo Vesala, and Sophia Walther
Earth Syst. Sci. Data, 15, 4295–4370, https://doi.org/10.5194/essd-15-4295-2023, https://doi.org/10.5194/essd-15-4295-2023, 2023
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Accurate estimation of fluxes of carbon dioxide from the land surface is essential for understanding future impacts of greenhouse gas emissions on the climate system. A wide variety of methods currently exist to estimate these sources and sinks. We are continuing work to develop annual comparisons of these diverse methods in order to clarify what they all actually calculate and to resolve apparent disagreement, in addition to highlighting opportunities for increased understanding.
Tim René de Groot, Anne Margriet Mol, Katherine Mesdag, Pierre Ramond, Rachel Ndhlovu, Julia Catherine Engelmann, Thomas Röckmann, and Helge Niemann
Biogeosciences, 20, 3857–3872, https://doi.org/10.5194/bg-20-3857-2023, https://doi.org/10.5194/bg-20-3857-2023, 2023
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This study investigates methane dynamics in the Wadden Sea. Our measurements revealed distinct variations triggered by seasonality and tidal forcing. The methane budget was higher in warmer seasons but surprisingly high in colder seasons. Methane dynamics were amplified during low tides, flushing the majority of methane into the North Sea or releasing it to the atmosphere. Methanotrophic activity was also elevated during low tide but mitigated only a small fraction of the methane efflux.
Foteini Stavropoulou, Katarina Vinković, Bert Kers, Marcel de Vries, Steven van Heuven, Piotr Korbeń, Martina Schmidt, Julia Wietzel, Pawel Jagoda, Jaroslav M. Necki, Jakub Bartyzel, Hossein Maazallahi, Malika Menoud, Carina van der Veen, Sylvia Walter, Béla Tuzson, Jonas Ravelid, Randulph Paulo Morales, Lukas Emmenegger, Dominik Brunner, Michael Steiner, Arjan Hensen, Ilona Velzeboer, Pim van den Bulk, Hugo Denier van der Gon, Antonio Delre, Maklawe Essonanawe Edjabou, Charlotte Scheutz, Marius Corbu, Sebastian Iancu, Denisa Moaca, Alin Scarlat, Alexandru Tudor, Ioana Vizireanu, Andreea Calcan, Magdalena Ardelean, Sorin Ghemulet, Alexandru Pana, Aurel Constantinescu, Lucian Cusa, Alexandru Nica, Calin Baciu, Cristian Pop, Andrei Radovici, Alexandru Mereuta, Horatiu Stefanie, Alexandru Dandocsi, Bas Hermans, Stefan Schwietzke, Daniel Zavala-Araiza, Huilin Chen, and Thomas Röckmann
Atmos. Chem. Phys., 23, 10399–10412, https://doi.org/10.5194/acp-23-10399-2023, https://doi.org/10.5194/acp-23-10399-2023, 2023
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In this study, we quantify CH4 emissions from onshore oil production sites in Romania at source and facility level using a combination of ground- and drone-based measurement techniques. We show that the total CH4 emissions in our studied areas are much higher than the emissions reported to UNFCCC, and up to three-quarters of the detected emissions are related to operational venting. Our results suggest that oil and gas production infrastructure in Romania holds a massive mitigation potential.
Berend J. Schuit, Joannes D. Maasakkers, Pieter Bijl, Gourav Mahapatra, Anne-Wil van den Berg, Sudhanshu Pandey, Alba Lorente, Tobias Borsdorff, Sander Houweling, Daniel J. Varon, Jason McKeever, Dylan Jervis, Marianne Girard, Itziar Irakulis-Loitxate, Javier Gorroño, Luis Guanter, Daniel H. Cusworth, and Ilse Aben
Atmos. Chem. Phys., 23, 9071–9098, https://doi.org/10.5194/acp-23-9071-2023, https://doi.org/10.5194/acp-23-9071-2023, 2023
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Using two machine learning models, which were trained on TROPOMI methane satellite data, we detect 2974 methane plumes, so-called super-emitters, in 2021. We detect methane emissions globally related to urban areas or landfills, coal mining, and oil and gas production. Using our monitoring system, we identify 94 regions with frequent emissions. For 12 locations, we target high-resolution satellite instruments to enlarge and identify the exact infrastructure responsible for the emissions.
Sara M. Defratyka, James L. France, Rebecca E. Fisher, Dave Lowry, Julianne M. Fernandez, Semra Bakkaloglu, Camille Yver-Kwok, Jean-Daniel Paris, Philippe Bousquet, Tim Arnold, Chris Rennick, Jon Helmore, Nigel Yarrow, and Euan G. Nisbet
EGUsphere, https://doi.org/10.5194/egusphere-2023-1490, https://doi.org/10.5194/egusphere-2023-1490, 2023
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We are focused on verification of δ13CH4 measurements in near-source conditions and we have provided an insight into the impact of chosen calculation methods for determined isotopic signatures. Our study offers a step forward for establishing an unified, robust, and reliable analytical technique to determine δ13CH4 of methane sources. Our recommended analytical approach reduces biases and uncertainties coming from measurement conditions, data clustering and various available fitting methods.
Sune Olander Rasmussen, Dorthe Dahl-Jensen, Hubertus Fischer, Katrin Fuhrer, Steffen Bo Hansen, Margareta Hansson, Christine S. Hvidberg, Ulf Jonsell, Sepp Kipfstuhl, Urs Ruth, Jakob Schwander, Marie-Louise Siggaard-Andersen, Giulia Sinnl, Jørgen Peder Steffensen, Anders M. Svensson, and Bo M. Vinther
Earth Syst. Sci. Data, 15, 3351–3364, https://doi.org/10.5194/essd-15-3351-2023, https://doi.org/10.5194/essd-15-3351-2023, 2023
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Timescales are essential for interpreting palaeoclimate data. The data series presented here were used for annual-layer identification when constructing the timescales named the Greenland Ice-Core Chronology 2005 (GICC05) and the revised version GICC21. Hopefully, these high-resolution data sets will be useful also for other purposes.
Andreas Forstmaier, Jia Chen, Florian Dietrich, Juan Bettinelli, Hossein Maazallahi, Carsten Schneider, Dominik Winkler, Xinxu Zhao, Taylor Jones, Carina van der Veen, Norman Wildmann, Moritz Makowski, Aydin Uzun, Friedrich Klappenbach, Hugo Denier van der Gon, Stefan Schwietzke, and Thomas Röckmann
Atmos. Chem. Phys., 23, 6897–6922, https://doi.org/10.5194/acp-23-6897-2023, https://doi.org/10.5194/acp-23-6897-2023, 2023
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Large cities emit greenhouse gases which contribute to global warming. In this study, we measured the release of one important green house gas, methane, in Hamburg. Multiple sources that contribute to methane emissions were located and quantified. Methane sources were found to be mainly caused by human activity (e.g., by release from oil and gas refineries). Moreover, potential natural sources have been located, such as the Elbe River and lakes.
Michaela Mühl, Jochen Schmitt, Barbara Seth, James E. Lee, Jon S. Edwards, Edward J. Brook, Thomas Blunier, and Hubertus Fischer
Clim. Past, 19, 999–1025, https://doi.org/10.5194/cp-19-999-2023, https://doi.org/10.5194/cp-19-999-2023, 2023
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Our ice core measurements show that methane, ethane, and propane concentrations are significantly elevated above their past atmospheric background for Greenland ice samples containing mineral dust. The underlying co-production process happens during the classical discrete wet extraction of air from the ice sample and affects previous reconstructions of the inter-polar difference of methane as well as methane stable isotope records derived from dust-rich Greenland ice.
Truls Andersen, Zhao Zhao, Marcel de Vries, Jaroslaw Necki, Justyna Swolkien, Malika Menoud, Thomas Röckmann, Anke Roiger, Andreas Fix, Wouter Peters, and Huilin Chen
Atmos. Chem. Phys., 23, 5191–5216, https://doi.org/10.5194/acp-23-5191-2023, https://doi.org/10.5194/acp-23-5191-2023, 2023
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The Upper Silesian Coal Basin, Poland, is one of the hot spots of methane emissions in Europe. Using an uncrewed aerial vehicle (UAV), we performed atmospheric measurements of methane concentrations downwind of five ventilation shafts in this region and determined the emission rates from the individual shafts. We found a strong correlation between quantified shaft-averaged emission rates and hourly inventory data, which also allows us to estimate the methane emissions from the entire region.
Robert Mulvaney, Eric W. Wolff, Mackenzie M. Grieman, Helene H. Hoffmann, Jack D. Humby, Christoph Nehrbass-Ahles, Rachael H. Rhodes, Isobel F. Rowell, Frédéric Parrenin, Loïc Schmidely, Hubertus Fischer, Thomas F. Stocker, Marcus Christl, Raimund Muscheler, Amaelle Landais, and Frédéric Prié
Clim. Past, 19, 851–864, https://doi.org/10.5194/cp-19-851-2023, https://doi.org/10.5194/cp-19-851-2023, 2023
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We present an age scale for a new ice core drilled at Skytrain Ice Rise, an ice rise facing the Ronne Ice Shelf in Antarctica. Various measurements in the ice and air phases are used to match the ice core to other Antarctic cores that have already been dated, and a new age scale is constructed. The 651 m ice core includes ice that is confidently dated to 117 000–126 000 years ago, in the last interglacial. Older ice is found deeper down, but there are flow disturbances in the deeper ice.
Ana Maria Roxana Petrescu, Chunjing Qiu, Matthew J. McGrath, Philippe Peylin, Glen P. Peters, Philippe Ciais, Rona L. Thompson, Aki Tsuruta, Dominik Brunner, Matthias Kuhnert, Bradley Matthews, Paul I. Palmer, Oksana Tarasova, Pierre Regnier, Ronny Lauerwald, David Bastviken, Lena Höglund-Isaksson, Wilfried Winiwarter, Giuseppe Etiope, Tuula Aalto, Gianpaolo Balsamo, Vladislav Bastrikov, Antoine Berchet, Patrick Brockmann, Giancarlo Ciotoli, Giulia Conchedda, Monica Crippa, Frank Dentener, Christine D. Groot Zwaaftink, Diego Guizzardi, Dirk Günther, Jean-Matthieu Haussaire, Sander Houweling, Greet Janssens-Maenhout, Massaer Kouyate, Adrian Leip, Antti Leppänen, Emanuele Lugato, Manon Maisonnier, Alistair J. Manning, Tiina Markkanen, Joe McNorton, Marilena Muntean, Gabriel D. Oreggioni, Prabir K. Patra, Lucia Perugini, Isabelle Pison, Maarit T. Raivonen, Marielle Saunois, Arjo J. Segers, Pete Smith, Efisio Solazzo, Hanqin Tian, Francesco N. Tubiello, Timo Vesala, Guido R. van der Werf, Chris Wilson, and Sönke Zaehle
Earth Syst. Sci. Data, 15, 1197–1268, https://doi.org/10.5194/essd-15-1197-2023, https://doi.org/10.5194/essd-15-1197-2023, 2023
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This study updates the state-of-the-art scientific overview of CH4 and N2O emissions in the EU27 and UK in Petrescu et al. (2021a). Yearly updates are needed to improve the different respective approaches and to inform on the development of formal verification systems. It integrates the most recent emission inventories, process-based model and regional/global inversions, comparing them with UNFCCC national GHG inventories, in support to policy to facilitate real-time verification procedures.
Saqr Munassar, Guillaume Monteil, Marko Scholze, Ute Karstens, Christian Rödenbeck, Frank-Thomas Koch, Kai U. Totsche, and Christoph Gerbig
Atmos. Chem. Phys., 23, 2813–2828, https://doi.org/10.5194/acp-23-2813-2023, https://doi.org/10.5194/acp-23-2813-2023, 2023
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Using different transport models results in large errors in optimized fluxes in the atmospheric inversions. Boundary conditions and inversion system configurations lead to a smaller but non-negligible impact. The findings highlight the importance to validate transport models for further developments but also to properly account for such errors in inverse modelling. This will help narrow the convergence of gas estimates reported in the scientific literature from different inversion frameworks.
Dominik Brunner, Gerrit Kuhlmann, Stephan Henne, Erik Koene, Bastian Kern, Sebastian Wolff, Christiane Voigt, Patrick Jöckel, Christoph Kiemle, Anke Roiger, Alina Fiehn, Sven Krautwurst, Konstantin Gerilowski, Heinrich Bovensmann, Jakob Borchardt, Michal Galkowski, Christoph Gerbig, Julia Marshall, Andrzej Klonecki, Pascal Prunet, Robert Hanfland, Margit Pattantyús-Ábrahám, Andrzej Wyszogrodzki, and Andreas Fix
Atmos. Chem. Phys., 23, 2699–2728, https://doi.org/10.5194/acp-23-2699-2023, https://doi.org/10.5194/acp-23-2699-2023, 2023
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We evaluated six atmospheric transport models for their capability to simulate the CO2 plumes from two of the largest power plants in Europe by comparing the models against aircraft observations collected during the CoMet (Carbon Dioxide and Methane Mission) campaign in 2018. The study analyzed how realistically such plumes can be simulated at different model resolutions and how well the planned European satellite mission CO2M will be able to quantify emissions from power plants.
Lars Mächler, Daniel Baggenstos, Florian Krauss, Jochen Schmitt, Bernhard Bereiter, Remo Walther, Christoph Reinhard, Béla Tuzson, Lukas Emmenegger, and Hubertus Fischer
Atmos. Meas. Tech., 16, 355–372, https://doi.org/10.5194/amt-16-355-2023, https://doi.org/10.5194/amt-16-355-2023, 2023
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We present a new method to extract the gases from ice cores and measure their greenhouse gas composition. The ice is sublimated continuously with a near-infrared laser, releasing the gases, which are then analyzed on a laser absorption spectrometer. The main advantage over previous efforts is a low effective resolution of 1–2 cm. This capability is crucial for the analysis of highly thinned ice, as expected from ongoing drilling efforts to extend ice core history further back in time.
Srijana Lama, Sander Houweling, K. Folkert Boersma, Ilse Aben, Hugo A. C. Denier van der Gon, and Maarten C. Krol
Atmos. Chem. Phys., 22, 16053–16071, https://doi.org/10.5194/acp-22-16053-2022, https://doi.org/10.5194/acp-22-16053-2022, 2022
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Hydroxyl radical (OH) is the important chemical species that determines the lifetime of some greenhouse gases and trace gases. OH plays a vital role in air pollution chemistry. OH has a short lifetime and is extremely difficult to measure directly. OH concentrations derived from the chemistry transport model (CTM) have uncertainties of >50 %. Therefore, in this study, OH is derived indirectly using satellite date in urban plumes.
Bryce F. J. Kelly, Xinyi Lu, Stephen J. Harris, Bruno G. Neininger, Jorg M. Hacker, Stefan Schwietzke, Rebecca E. Fisher, James L. France, Euan G. Nisbet, David Lowry, Carina van der Veen, Malika Menoud, and Thomas Röckmann
Atmos. Chem. Phys., 22, 15527–15558, https://doi.org/10.5194/acp-22-15527-2022, https://doi.org/10.5194/acp-22-15527-2022, 2022
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This study explores using the composition of methane of in-flight atmospheric air samples for greenhouse gas inventory verification. The air samples were collected above one of the largest coal seam gas production regions in the world. Adjacent to these gas fields are coal mines, Australia's largest cattle feedlot, and over 1 million grazing cattle. The results are also used to identify methane mitigation opportunities.
Sourish Basu, Xin Lan, Edward Dlugokencky, Sylvia Michel, Stefan Schwietzke, John B. Miller, Lori Bruhwiler, Youmi Oh, Pieter P. Tans, Francesco Apadula, Luciana V. Gatti, Armin Jordan, Jaroslaw Necki, Motoki Sasakawa, Shinji Morimoto, Tatiana Di Iorio, Haeyoung Lee, Jgor Arduini, and Giovanni Manca
Atmos. Chem. Phys., 22, 15351–15377, https://doi.org/10.5194/acp-22-15351-2022, https://doi.org/10.5194/acp-22-15351-2022, 2022
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Atmospheric methane (CH4) has been growing steadily since 2007 for reasons that are not well understood. Here we determine sources of methane using a technique informed by atmospheric measurements of CH4 and its isotopologue 13CH4. Measurements of 13CH4 provide for better separation of microbial, fossil, and fire sources of methane than CH4 measurements alone. Compared to previous assessments such as the Global Carbon Project, we find a larger microbial contribution to the post-2007 increase.
Prabhakar Shrestha, Jana Mendrok, and Dominik Brunner
Atmos. Chem. Phys., 22, 14095–14117, https://doi.org/10.5194/acp-22-14095-2022, https://doi.org/10.5194/acp-22-14095-2022, 2022
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The study extends the Terrestrial Systems Modeling Platform with gas-phase chemistry aerosol dynamics and a radar forward operator to enable detailed studies of aerosol–cloud–precipitation interactions. This is demonstrated using a case study of a deep convective storm, which showed that the strong updraft in the convective core of the storm produced aerosol-tower-like features, which affected the size of the hydrometeors and the simulated polarimetric features (e.g., ZDR and KDP columns).
Peter Bergamaschi, Arjo Segers, Dominik Brunner, Jean-Matthieu Haussaire, Stephan Henne, Michel Ramonet, Tim Arnold, Tobias Biermann, Huilin Chen, Sebastien Conil, Marc Delmotte, Grant Forster, Arnoud Frumau, Dagmar Kubistin, Xin Lan, Markus Leuenberger, Matthias Lindauer, Morgan Lopez, Giovanni Manca, Jennifer Müller-Williams, Simon O'Doherty, Bert Scheeren, Martin Steinbacher, Pamela Trisolino, Gabriela Vítková, and Camille Yver Kwok
Atmos. Chem. Phys., 22, 13243–13268, https://doi.org/10.5194/acp-22-13243-2022, https://doi.org/10.5194/acp-22-13243-2022, 2022
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We present a novel high-resolution inverse modelling system, "FLEXVAR", and its application for the inverse modelling of European CH4 emissions in 2018. The new system combines a high spatial resolution of 7 km x 7 km with a variational data assimilation technique, which allows CH4 emissions to be optimized from individual model grid cells. The high resolution allows the observations to be better reproduced, while the derived emissions show overall good consistency with two existing models.
Malika Menoud, Carina van der Veen, Dave Lowry, Julianne M. Fernandez, Semra Bakkaloglu, James L. France, Rebecca E. Fisher, Hossein Maazallahi, Mila Stanisavljević, Jarosław Nęcki, Katarina Vinkovic, Patryk Łakomiec, Janne Rinne, Piotr Korbeń, Martina Schmidt, Sara Defratyka, Camille Yver-Kwok, Truls Andersen, Huilin Chen, and Thomas Röckmann
Earth Syst. Sci. Data, 14, 4365–4386, https://doi.org/10.5194/essd-14-4365-2022, https://doi.org/10.5194/essd-14-4365-2022, 2022
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Emission sources of methane (CH4) can be distinguished with measurements of CH4 stable isotopes. We present new measurements of isotope signatures of various CH4 sources in Europe, mainly anthropogenic, sampled from 2017 to 2020. The present database also contains the most recent update of the global signature dataset from the literature. The dataset improves CH4 source attribution and the understanding of the global CH4 budget.
Simone M. Pieber, Béla Tuzson, Stephan Henne, Ute Karstens, Christoph Gerbig, Frank-Thomas Koch, Dominik Brunner, Martin Steinbacher, and Lukas Emmenegger
Atmos. Chem. Phys., 22, 10721–10749, https://doi.org/10.5194/acp-22-10721-2022, https://doi.org/10.5194/acp-22-10721-2022, 2022
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Understanding regional greenhouse gas emissions into the atmosphere is a prerequisite to mitigate climate change. In this study, we investigated the regional contributions of carbon dioxide (CO2) at the location of the high Alpine observatory Jungfraujoch (JFJ, Switzerland, 3580 m a.s.l.). To this purpose, we combined receptor-oriented atmospheric transport simulations for CO2 concentration in the period 2009–2017 with stable carbon isotope (δ13C–CO2) information.
Qiansi Tu, Matthias Schneider, Frank Hase, Farahnaz Khosrawi, Benjamin Ertl, Jaroslaw Necki, Darko Dubravica, Christopher J. Diekmann, Thomas Blumenstock, and Dianjun Fang
Atmos. Chem. Phys., 22, 9747–9765, https://doi.org/10.5194/acp-22-9747-2022, https://doi.org/10.5194/acp-22-9747-2022, 2022
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Three-year satellite observations and high-resolution model forecast of XCH4 are used to derive CH4 emissions in the USCB region, Poland – a region of intense coal mining activities. The wind-assigned anomalies for two opposite wind directions are calculated and the estimated emission rates are very close to the inventories and in reasonable agreement with the previous studies. Our method is quite robust and can serve as a simple method to estimate CH4 or CO2 emissions for other regions.
Eric W. Wolff, Hubertus Fischer, Tas van Ommen, and David A. Hodell
Clim. Past, 18, 1563–1577, https://doi.org/10.5194/cp-18-1563-2022, https://doi.org/10.5194/cp-18-1563-2022, 2022
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Projects are underway to drill ice cores in Antarctica reaching 1.5 Myr back in time. Dating such cores will be challenging. One method is to match records from the new core against datasets from existing marine sediment cores. Here we explore the options for doing this and assess how well the ice and marine records match over the existing 800 000-year time period. We are able to recommend a strategy for using marine data to place an age scale on the new ice cores.
Sudhanshu Pandey, Sander Houweling, and Arjo Segers
Geosci. Model Dev., 15, 4555–4567, https://doi.org/10.5194/gmd-15-4555-2022, https://doi.org/10.5194/gmd-15-4555-2022, 2022
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Inversions are used to calculate methane emissions using atmospheric mole-fraction measurements. Multidecadal inversions are needed to extract information from the long measurement records of methane. However, multidecadal inversion computations can take months to finish. Here, we demonstrate an order of magnitude improvement in wall clock time for an iterative multidecadal inversion by physical parallelization of chemical transport model.
Andreas Luther, Julian Kostinek, Ralph Kleinschek, Sara Defratyka, Mila Stanisavljević, Andreas Forstmaier, Alexandru Dandocsi, Leon Scheidweiler, Darko Dubravica, Norman Wildmann, Frank Hase, Matthias M. Frey, Jia Chen, Florian Dietrich, Jarosław Nȩcki, Justyna Swolkień, Christoph Knote, Sanam N. Vardag, Anke Roiger, and André Butz
Atmos. Chem. Phys., 22, 5859–5876, https://doi.org/10.5194/acp-22-5859-2022, https://doi.org/10.5194/acp-22-5859-2022, 2022
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Coal mining is an extensive source of anthropogenic methane emissions. In order to reduce and mitigate methane emissions, it is important to know how much and where the methane is emitted. We estimated coal mining methane emissions in Poland based on atmospheric methane measurements and particle dispersion modeling. In general, our emission estimates suggest higher emissions than expected by previous annual emission reports.
Carlos Alberti, Frank Hase, Matthias Frey, Darko Dubravica, Thomas Blumenstock, Angelika Dehn, Paolo Castracane, Gregor Surawicz, Roland Harig, Bianca C. Baier, Caroline Bès, Jianrong Bi, Hartmut Boesch, André Butz, Zhaonan Cai, Jia Chen, Sean M. Crowell, Nicholas M. Deutscher, Dragos Ene, Jonathan E. Franklin, Omaira García, David Griffith, Bruno Grouiez, Michel Grutter, Abdelhamid Hamdouni, Sander Houweling, Neil Humpage, Nicole Jacobs, Sujong Jeong, Lilian Joly, Nicholas B. Jones, Denis Jouglet, Rigel Kivi, Ralph Kleinschek, Morgan Lopez, Diogo J. Medeiros, Isamu Morino, Nasrin Mostafavipak, Astrid Müller, Hirofumi Ohyama, Paul I. Palmer, Mahesh Pathakoti, David F. Pollard, Uwe Raffalski, Michel Ramonet, Robbie Ramsay, Mahesh Kumar Sha, Kei Shiomi, William Simpson, Wolfgang Stremme, Youwen Sun, Hiroshi Tanimoto, Yao Té, Gizaw Mengistu Tsidu, Voltaire A. Velazco, Felix Vogel, Masataka Watanabe, Chong Wei, Debra Wunch, Marcia Yamasoe, Lu Zhang, and Johannes Orphal
Atmos. Meas. Tech., 15, 2433–2463, https://doi.org/10.5194/amt-15-2433-2022, https://doi.org/10.5194/amt-15-2433-2022, 2022
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Space-borne greenhouse gas missions require ground-based validation networks capable of providing fiducial reference measurements. Here, considerable refinements of the calibration procedures for the COllaborative Carbon Column Observing Network (COCCON) are presented. Laboratory and solar side-by-side procedures for the characterization of the spectrometers have been refined and extended. Revised calibration factors for XCO2, XCO and XCH4 are provided, incorporating 47 new spectrometers.
Randulph Morales, Jonas Ravelid, Katarina Vinkovic, Piotr Korbeń, Béla Tuzson, Lukas Emmenegger, Huilin Chen, Martina Schmidt, Sebastian Humbel, and Dominik Brunner
Atmos. Meas. Tech., 15, 2177–2198, https://doi.org/10.5194/amt-15-2177-2022, https://doi.org/10.5194/amt-15-2177-2022, 2022
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Mapping trace gas emission plumes using in situ measurements from unmanned aerial vehicles (UAVs) is an emerging and attractive possibility to quantify emissions from localized sources. We performed an extensive controlled-release experiment to develop an optimal quantification method and to determine the related uncertainties under various environmental and sampling conditions. Our approach was successful in quantifying local methane sources from drone-based measurements.
Amy Foulds, Grant Allen, Jacob T. Shaw, Prudence Bateson, Patrick A. Barker, Langwen Huang, Joseph R. Pitt, James D. Lee, Shona E. Wilde, Pamela Dominutti, Ruth M. Purvis, David Lowry, James L. France, Rebecca E. Fisher, Alina Fiehn, Magdalena Pühl, Stéphane J. B. Bauguitte, Stephen A. Conley, Mackenzie L. Smith, Tom Lachlan-Cope, Ignacio Pisso, and Stefan Schwietzke
Atmos. Chem. Phys., 22, 4303–4322, https://doi.org/10.5194/acp-22-4303-2022, https://doi.org/10.5194/acp-22-4303-2022, 2022
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We measured CH4 emissions from 21 offshore oil and gas facilities in the Norwegian Sea in 2019. Measurements compared well with operator-reported emissions but were greatly underestimated when compared with a 2016 global fossil fuel inventory. This study demonstrates the need for up-to-date and accurate inventories for use in research and policy and the important benefits of best-practice reporting methods by operators. Airborne measurements are an effective tool to validate such inventories.
Gerrit Kuhlmann, Ka Lok Chan, Sebastian Donner, Ying Zhu, Marc Schwaerzel, Steffen Dörner, Jia Chen, Andreas Hueni, Duc Hai Nguyen, Alexander Damm, Annette Schütt, Florian Dietrich, Dominik Brunner, Cheng Liu, Brigitte Buchmann, Thomas Wagner, and Mark Wenig
Atmos. Meas. Tech., 15, 1609–1629, https://doi.org/10.5194/amt-15-1609-2022, https://doi.org/10.5194/amt-15-1609-2022, 2022
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Nitrogen dioxide (NO2) is an air pollutant whose concentration often exceeds air quality guideline values, especially in urban areas. To map the spatial distribution of NO2 in Munich, we conducted the Munich NO2 Imaging Campaign (MuNIC), where NO2 was measured with stationary, mobile, and airborne in situ and remote sensing instruments. The campaign provides a unique dataset that has been used to compare the different instruments and to study the spatial variability of NO2 and its sources.
Eric Saboya, Giulia Zazzeri, Heather Graven, Alistair J. Manning, and Sylvia Englund Michel
Atmos. Chem. Phys., 22, 3595–3613, https://doi.org/10.5194/acp-22-3595-2022, https://doi.org/10.5194/acp-22-3595-2022, 2022
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Continuous measurements of atmospheric methane concentrations and its carbon-13 isotope have been made in central London since early 2018. These measurements were used to evaluate methane emissions reported in global and UK-specific emission inventories for the London area. Compared to atmospheric methane measurements from March 2018 to October 2020, both inventories are under-reporting natural gas leakage for the London area.
Tobias Erhardt, Matthias Bigler, Urs Federer, Gideon Gfeller, Daiana Leuenberger, Olivia Stowasser, Regine Röthlisberger, Simon Schüpbach, Urs Ruth, Birthe Twarloh, Anna Wegner, Kumiko Goto-Azuma, Takayuki Kuramoto, Helle A. Kjær, Paul T. Vallelonga, Marie-Louise Siggaard-Andersen, Margareta E. Hansson, Ailsa K. Benton, Louise G. Fleet, Rob Mulvaney, Elizabeth R. Thomas, Nerilie Abram, Thomas F. Stocker, and Hubertus Fischer
Earth Syst. Sci. Data, 14, 1215–1231, https://doi.org/10.5194/essd-14-1215-2022, https://doi.org/10.5194/essd-14-1215-2022, 2022
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The datasets presented alongside this manuscript contain high-resolution concentration measurements of chemical impurities in deep ice cores, NGRIP and NEEM, from the Greenland ice sheet. The impurities originate from the deposition of aerosols to the surface of the ice sheet and are influenced by source, transport and deposition processes. Together, these records contain detailed, multi-parameter records of past climate variability over the last glacial period.
Jiamei Lin, Anders Svensson, Christine S. Hvidberg, Johannes Lohmann, Steffen Kristiansen, Dorthe Dahl-Jensen, Jørgen Peder Steffensen, Sune Olander Rasmussen, Eliza Cook, Helle Astrid Kjær, Bo M. Vinther, Hubertus Fischer, Thomas Stocker, Michael Sigl, Matthias Bigler, Mirko Severi, Rita Traversi, and Robert Mulvaney
Clim. Past, 18, 485–506, https://doi.org/10.5194/cp-18-485-2022, https://doi.org/10.5194/cp-18-485-2022, 2022
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We employ acidity records from Greenland and Antarctic ice cores to estimate the emission strength, frequency and climatic forcing for large volcanic eruptions from the last half of the last glacial period. A total of 25 volcanic eruptions are found to be larger than any eruption in the last 2500 years, and we identify more eruptions than obtained from geological evidence. Towards the end of the glacial period, there is a notable increase in volcanic activity observed for Greenland.
Stephen M. Platt, Øystein Hov, Torunn Berg, Knut Breivik, Sabine Eckhardt, Konstantinos Eleftheriadis, Nikolaos Evangeliou, Markus Fiebig, Rebecca Fisher, Georg Hansen, Hans-Christen Hansson, Jost Heintzenberg, Ove Hermansen, Dominic Heslin-Rees, Kim Holmén, Stephen Hudson, Roland Kallenborn, Radovan Krejci, Terje Krognes, Steinar Larssen, David Lowry, Cathrine Lund Myhre, Chris Lunder, Euan Nisbet, Pernilla B. Nizzetto, Ki-Tae Park, Christina A. Pedersen, Katrine Aspmo Pfaffhuber, Thomas Röckmann, Norbert Schmidbauer, Sverre Solberg, Andreas Stohl, Johan Ström, Tove Svendby, Peter Tunved, Kjersti Tørnkvist, Carina van der Veen, Stergios Vratolis, Young Jun Yoon, Karl Espen Yttri, Paul Zieger, Wenche Aas, and Kjetil Tørseth
Atmos. Chem. Phys., 22, 3321–3369, https://doi.org/10.5194/acp-22-3321-2022, https://doi.org/10.5194/acp-22-3321-2022, 2022
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Here we detail the history of the Zeppelin Observatory, a unique global background site and one of only a few in the high Arctic. We present long-term time series of up to 30 years of atmospheric components and atmospheric transport phenomena. Many of these time series are important to our understanding of Arctic and global atmospheric composition change. Finally, we discuss the future of the Zeppelin Observatory and emerging areas of future research on the Arctic atmosphere.
Roland Vernooij, Ulrike Dusek, Maria Elena Popa, Peng Yao, Anupam Shaikat, Chenxi Qiu, Patrik Winiger, Carina van der Veen, Thomas Callum Eames, Natasha Ribeiro, and Guido R. van der Werf
Atmos. Chem. Phys., 22, 2871–2890, https://doi.org/10.5194/acp-22-2871-2022, https://doi.org/10.5194/acp-22-2871-2022, 2022
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Landscape fires are a major source of greenhouse gases and aerosols, particularly in sub-tropical savannas. Stable carbon isotopes in emissions can be used to trace the contribution of C3 plants (e.g. trees or shrubs) and C4 plants (e.g. savanna grasses) to greenhouse gases and aerosols if the process is well understood. This helps us to link individual vegetation types to emissions, identify biomass burning emissions in the atmosphere, and improve the reconstruction of historic fire regimes.
Yousef Albuhaisi, Ype van der Velde, and Sander Houweling
Biogeosciences Discuss., https://doi.org/10.5194/bg-2022-55, https://doi.org/10.5194/bg-2022-55, 2022
Manuscript not accepted for further review
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An important uncertainty in the modelling of methane emissions from natural wetlands is the wetland area. It is important to get the spatiotemporal covariance between the variables that drive methane emissions right for accurate quantification. Using high-resolution wetland and soil carbon maps, in combination with a simplified methane emission model that is coarsened in six steps from 0.005° to 1°, we find a strong relation between wetland emissions and the model resolution.
Dominique Rust, Ioannis Katharopoulos, Martin K. Vollmer, Stephan Henne, Simon O'Doherty, Daniel Say, Lukas Emmenegger, Renato Zenobi, and Stefan Reimann
Atmos. Chem. Phys., 22, 2447–2466, https://doi.org/10.5194/acp-22-2447-2022, https://doi.org/10.5194/acp-22-2447-2022, 2022
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Artificial halocarbons contribute to ozone layer depletion and to global warming. We measured the atmospheric concentrations of halocarbons at the Beromünster tower, modelled the Swiss emissions, and compared the results to the internationally reported Swiss emissions inventory. For most of the halocarbons, we found good agreement, whereas one refrigerant might be overestimated in the inventory. In addition, we present first emission estimates of the newest types of halocarbons.
Juhi Nagori, Narcisa Nechita-Bândă, Sebastian Oscar Danielache, Masumi Shinkai, Thomas Röckmann, and Maarten Krol
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-68, https://doi.org/10.5194/acp-2022-68, 2022
Publication in ACP not foreseen
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The sulfur isotopes (32S and 34S) were studied to understand the sources, sinks and processes of carbonyl sulphide (COS) in the atmosphere. COS is an important source of sulfur aerosol in the stratosphere (SSA). Few measurements of COS and SSA exist, but with our 1D model, we were able to match them and show the importance of COS to sulfate formation. Moreover, we are able to highlight some important processes for the COS budget and where measurements may fill a gap in current knowledge.
Sven Krautwurst, Konstantin Gerilowski, Jakob Borchardt, Norman Wildmann, Michał Gałkowski, Justyna Swolkień, Julia Marshall, Alina Fiehn, Anke Roiger, Thomas Ruhtz, Christoph Gerbig, Jaroslaw Necki, John P. Burrows, Andreas Fix, and Heinrich Bovensmann
Atmos. Chem. Phys., 21, 17345–17371, https://doi.org/10.5194/acp-21-17345-2021, https://doi.org/10.5194/acp-21-17345-2021, 2021
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Quantification of anthropogenic CH4 emissions remains challenging, but it is essential for near-term climate mitigation strategies. We use airborne remote sensing observations to assess bottom-up estimates of coal mining emissions from one of Europe's largest CH4 emission hot spots located in Poland. The analysis reveals that emissions from small groups of shafts can be disentangled, but caution is advised when comparing observations to commonly reported annual emissions.
Vilma Kangasaho, Aki Tsuruta, Leif Backman, Pyry Mäkinen, Sander Houweling, Arjo Segers, Maarten Krol, Ed Dlugokencky, Sylvia Michel, James White, and Tuula Aalto
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-843, https://doi.org/10.5194/acp-2021-843, 2021
Revised manuscript not accepted
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Understanding the composition of carbon isotopes can help to better understand the changes in methane budgets. This study investigates how methane sources affect the seasonal cycle of the methane carbon-13 isotope during 2000–2012 using an atmospheric transport model. We found that emissions from both anthropogenic and natural sources contribute. The findings raise a need to revise the magnitudes, proportion, and seasonal cycles of anthropogenic sources and northern wetland emissions.
Marc Schwaerzel, Dominik Brunner, Fabian Jakub, Claudia Emde, Brigitte Buchmann, Alexis Berne, and Gerrit Kuhlmann
Atmos. Meas. Tech., 14, 6469–6482, https://doi.org/10.5194/amt-14-6469-2021, https://doi.org/10.5194/amt-14-6469-2021, 2021
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NO2 maps from airborne imaging remote sensing often appear much smoother than one would expect from high-resolution model simulations of NO2 over cities, despite the small ground-pixel size of the sensors. Our case study over Zurich, using the newly implemented building module of the MYSTIC radiative transfer solver, shows that the 3D effect can explain part of the smearing and that building shadows cause a noticeable underestimation and noise in the measured NO2 columns.
Anna K. Tobler, Alicja Skiba, Francesco Canonaco, Griša Močnik, Pragati Rai, Gang Chen, Jakub Bartyzel, Miroslaw Zimnoch, Katarzyna Styszko, Jaroslaw Nęcki, Markus Furger, Kazimierz Różański, Urs Baltensperger, Jay G. Slowik, and Andre S. H. Prevot
Atmos. Chem. Phys., 21, 14893–14906, https://doi.org/10.5194/acp-21-14893-2021, https://doi.org/10.5194/acp-21-14893-2021, 2021
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Kraków is among the cities with the highest particulate matter levels within Europe. We conducted long-term and highly time-resolved measurements of the chemical composition of submicron particlulate matter (PM1). Combined with advanced source apportionment techniques, which allow for time-dependent factor profiles, our results elucidate that traffic and residential heating (biomass burning and coal combustion) as well as oxygenated organic aerosol are the key PM sources in Kraków.
Malika Menoud, Carina van der Veen, Jaroslaw Necki, Jakub Bartyzel, Barbara Szénási, Mila Stanisavljević, Isabelle Pison, Philippe Bousquet, and Thomas Röckmann
Atmos. Chem. Phys., 21, 13167–13185, https://doi.org/10.5194/acp-21-13167-2021, https://doi.org/10.5194/acp-21-13167-2021, 2021
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Using measurements of methane isotopes in ambient air and a 3D atmospheric transport model, in Krakow, Poland, we mainly detected fossil-fuel-related sources, coming from coal mining in Silesia and from the use of natural gas in the city. Emission inventories report large emissions from coal mine activity in Silesia, which is in agreement with our measurements. However, methane sources in the urban area of Krakow related to the use of fossil fuels might be underestimated in the inventories.
Antoine Berchet, Espen Sollum, Rona L. Thompson, Isabelle Pison, Joël Thanwerdas, Grégoire Broquet, Frédéric Chevallier, Tuula Aalto, Adrien Berchet, Peter Bergamaschi, Dominik Brunner, Richard Engelen, Audrey Fortems-Cheiney, Christoph Gerbig, Christine D. Groot Zwaaftink, Jean-Matthieu Haussaire, Stephan Henne, Sander Houweling, Ute Karstens, Werner L. Kutsch, Ingrid T. Luijkx, Guillaume Monteil, Paul I. Palmer, Jacob C. A. van Peet, Wouter Peters, Philippe Peylin, Elise Potier, Christian Rödenbeck, Marielle Saunois, Marko Scholze, Aki Tsuruta, and Yuanhong Zhao
Geosci. Model Dev., 14, 5331–5354, https://doi.org/10.5194/gmd-14-5331-2021, https://doi.org/10.5194/gmd-14-5331-2021, 2021
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We present here the Community Inversion Framework (CIF) to help rationalize development efforts and leverage the strengths of individual inversion systems into a comprehensive framework. The CIF is a programming protocol to allow various inversion bricks to be exchanged among researchers.
The ensemble of bricks makes a flexible, transparent and open-source Python-based tool. We describe the main structure and functionalities and demonstrate it in a simple academic case.
Johannes Sutter, Hubertus Fischer, and Olaf Eisen
The Cryosphere, 15, 3839–3860, https://doi.org/10.5194/tc-15-3839-2021, https://doi.org/10.5194/tc-15-3839-2021, 2021
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Projections of global sea-level changes in a warming world require ice-sheet models. We expand the calibration of these models by making use of the internal architecture of the Antarctic ice sheet, which is formed by its evolution over many millennia. We propose that using our novel approach to constrain ice sheet models, we will be able to both sharpen our understanding of past and future sea-level changes and identify weaknesses in the parameterisation of current continental-scale models.
Ruth E. Hill-Pearce, Aimee Hillier, Eric Mussell Webber, Kanokrat Charoenpornpukdee, Simon O'Doherty, Joachim Mohn, Christoph Zellweger, David R. Worton, and Paul J. Brewer
Atmos. Meas. Tech., 14, 5447–5458, https://doi.org/10.5194/amt-14-5447-2021, https://doi.org/10.5194/amt-14-5447-2021, 2021
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There is currently a need for gas reference materials with well-characterised delta values for monitoring N2O amount fractions. We present work towards the preparation of gas reference materials for calibration of in-field monitoring equipment, which target the WMO-GAW data quality objectives for comparability of amount fraction and demonstrate the stability of δ15Nα, δ15Nβ and δ18O values with pressure and effects of cylinder passivation.
Loïc Schmidely, Christoph Nehrbass-Ahles, Jochen Schmitt, Juhyeong Han, Lucas Silva, Jinwha Shin, Fortunat Joos, Jérôme Chappellaz, Hubertus Fischer, and Thomas F. Stocker
Clim. Past, 17, 1627–1643, https://doi.org/10.5194/cp-17-1627-2021, https://doi.org/10.5194/cp-17-1627-2021, 2021
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Using ancient gas trapped in polar glaciers, we reconstructed the atmospheric concentrations of methane and nitrous oxide over the penultimate deglaciation to study their response to major climate changes. We show this deglaciation to be characterized by modes of methane and nitrous oxide variability that are also found during the last deglaciation and glacial cycle.
Xinyi Lu, Stephen J. Harris, Rebecca E. Fisher, James L. France, Euan G. Nisbet, David Lowry, Thomas Röckmann, Carina van der Veen, Malika Menoud, Stefan Schwietzke, and Bryce F. J. Kelly
Atmos. Chem. Phys., 21, 10527–10555, https://doi.org/10.5194/acp-21-10527-2021, https://doi.org/10.5194/acp-21-10527-2021, 2021
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Many coal seam gas (CSG) facilities in the Surat Basin, Australia, are adjacent to other sources of methane, including agricultural, urban, and natural seeps. This makes it challenging to estimate the amount of methane being emitted into the atmosphere from CSG facilities. This research demonstrates that measurements of the carbon and hydrogen stable isotopic composition of methane can distinguish between and apportion methane emissions from CSG facilities, cattle, and many other sources.
Guillaume Monteil and Marko Scholze
Geosci. Model Dev., 14, 3383–3406, https://doi.org/10.5194/gmd-14-3383-2021, https://doi.org/10.5194/gmd-14-3383-2021, 2021
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LUMIA is a Python library for atmospheric inversions, originally developed at Lund University to perform regional atmospheric CO2 inversions. The inversions rely on coupling the regional transport model FLEXPART and the global transport model TM5. The paper presents the modeling setup and some first results, and it introduces the LUMIA Python package as a toolbox for inversions beyond the use case presented in the paper.
Ana Maria Roxana Petrescu, Chunjing Qiu, Philippe Ciais, Rona L. Thompson, Philippe Peylin, Matthew J. McGrath, Efisio Solazzo, Greet Janssens-Maenhout, Francesco N. Tubiello, Peter Bergamaschi, Dominik Brunner, Glen P. Peters, Lena Höglund-Isaksson, Pierre Regnier, Ronny Lauerwald, David Bastviken, Aki Tsuruta, Wilfried Winiwarter, Prabir K. Patra, Matthias Kuhnert, Gabriel D. Oreggioni, Monica Crippa, Marielle Saunois, Lucia Perugini, Tiina Markkanen, Tuula Aalto, Christine D. Groot Zwaaftink, Hanqin Tian, Yuanzhi Yao, Chris Wilson, Giulia Conchedda, Dirk Günther, Adrian Leip, Pete Smith, Jean-Matthieu Haussaire, Antti Leppänen, Alistair J. Manning, Joe McNorton, Patrick Brockmann, and Albertus Johannes Dolman
Earth Syst. Sci. Data, 13, 2307–2362, https://doi.org/10.5194/essd-13-2307-2021, https://doi.org/10.5194/essd-13-2307-2021, 2021
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This study is topical and provides a state-of-the-art scientific overview of data availability from bottom-up and top-down CH4 and N2O emissions in the EU27 and UK. The data integrate recent emission inventories with process-based model data and regional/global inversions for the European domain, aiming at reconciling them with official country-level UNFCCC national GHG inventories in support to policy and to facilitate real-time verification procedures.
Ana Maria Roxana Petrescu, Matthew J. McGrath, Robbie M. Andrew, Philippe Peylin, Glen P. Peters, Philippe Ciais, Gregoire Broquet, Francesco N. Tubiello, Christoph Gerbig, Julia Pongratz, Greet Janssens-Maenhout, Giacomo Grassi, Gert-Jan Nabuurs, Pierre Regnier, Ronny Lauerwald, Matthias Kuhnert, Juraj Balkovič, Mart-Jan Schelhaas, Hugo A. C. Denier van der
Gon, Efisio Solazzo, Chunjing Qiu, Roberto Pilli, Igor B. Konovalov, Richard A. Houghton, Dirk Günther, Lucia Perugini, Monica Crippa, Raphael Ganzenmüller, Ingrid T. Luijkx, Pete Smith, Saqr Munassar, Rona L. Thompson, Giulia Conchedda, Guillaume Monteil, Marko Scholze, Ute Karstens, Patrick Brockmann, and Albertus Johannes Dolman
Earth Syst. Sci. Data, 13, 2363–2406, https://doi.org/10.5194/essd-13-2363-2021, https://doi.org/10.5194/essd-13-2363-2021, 2021
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This study is topical and provides a state-of-the-art scientific overview of data availability from bottom-up and top-down CO2 fossil emissions and CO2 land fluxes in the EU27+UK. The data integrate recent emission inventories with ecosystem data, land carbon models and regional/global inversions for the European domain, aiming at reconciling CO2 estimates with official country-level UNFCCC national GHG inventories in support to policy and facilitating real-time verification procedures.
Max Thomas, Johannes C. Laube, Jan Kaiser, Samuel Allin, Patricia Martinerie, Robert Mulvaney, Anna Ridley, Thomas Röckmann, William T. Sturges, and Emmanuel Witrant
Atmos. Chem. Phys., 21, 6857–6873, https://doi.org/10.5194/acp-21-6857-2021, https://doi.org/10.5194/acp-21-6857-2021, 2021
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CFC gases are destroying the Earth's life-protecting ozone layer. We improve understanding of CFC destruction by measuring the isotopic fingerprint of the carbon in the three most abundant CFCs. These are the first such measurements in the main region where CFCs are destroyed – the stratosphere. We reconstruct the atmospheric isotope histories of these CFCs back to the 1950s by measuring air extracted from deep snow and using a model. The model and the measurements are generally consistent.
Marcel Haeberli, Daniel Baggenstos, Jochen Schmitt, Markus Grimmer, Adrien Michel, Thomas Kellerhals, and Hubertus Fischer
Clim. Past, 17, 843–867, https://doi.org/10.5194/cp-17-843-2021, https://doi.org/10.5194/cp-17-843-2021, 2021
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Using the temperature-dependent solubility of noble gases in ocean water, we reconstruct global mean ocean temperature (MOT) over the last 700 kyr using noble gas ratios in air enclosed in polar ice cores. Our record shows that glacial MOT was about 3 °C cooler compared to the Holocene. Interglacials before 450 kyr ago were characterized by about 1.5 °C lower MOT than the Holocene. In addition, some interglacials show transient maxima in ocean temperature related to changes in ocean circulation.
Stuart K. Grange, James D. Lee, Will S. Drysdale, Alastair C. Lewis, Christoph Hueglin, Lukas Emmenegger, and David C. Carslaw
Atmos. Chem. Phys., 21, 4169–4185, https://doi.org/10.5194/acp-21-4169-2021, https://doi.org/10.5194/acp-21-4169-2021, 2021
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The changes in mobility across Europe due to the COVID-19 lockdowns had consequences for air quality. We compare what was experienced to estimates of "what would have been" without the lockdowns. Nitrogen dioxide (NO2), an important vehicle-sourced pollutant, decreased by a third. However, ozone (O3) increased in response to lower NO2. Because NO2 is decreasing over time, increases in O3 can be expected in European urban areas and will require management to avoid future negative outcomes.
Manuel Graf, Philipp Scheidegger, André Kupferschmid, Herbert Looser, Thomas Peter, Ruud Dirksen, Lukas Emmenegger, and Béla Tuzson
Atmos. Meas. Tech., 14, 1365–1378, https://doi.org/10.5194/amt-14-1365-2021, https://doi.org/10.5194/amt-14-1365-2021, 2021
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Water vapor is the most important natural greenhouse gas. The accurate and frequent measurement of its abundance, especially in the upper troposphere and lower stratosphere (UTLS), is technically challenging. We developed and characterized a mid-IR absorption spectrometer for highly accurate water vapor measurements in the UTLS. The instrument is sufficiently small and lightweight (3.9 kg) to be carried by meteorological balloons, which enables frequent and cost-effective soundings.
Sudhanshu Pandey, Sander Houweling, Alba Lorente, Tobias Borsdorff, Maria Tsivlidou, A. Anthony Bloom, Benjamin Poulter, Zhen Zhang, and Ilse Aben
Biogeosciences, 18, 557–572, https://doi.org/10.5194/bg-18-557-2021, https://doi.org/10.5194/bg-18-557-2021, 2021
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We use atmospheric methane observations from the novel TROPOspheric Monitoring Instrument (TROPOMI; Sentinel-5p) to estimate methane emissions from South Sudan's wetlands. Our emission estimates are an order of magnitude larger than the estimate of process-based wetland models. We find that this underestimation by the models is likely due to their misrepresentation of the wetlands' inundation extent and temperature dependences.
Pragati Rai, Jay G. Slowik, Markus Furger, Imad El Haddad, Suzanne Visser, Yandong Tong, Atinderpal Singh, Günther Wehrle, Varun Kumar, Anna K. Tobler, Deepika Bhattu, Liwei Wang, Dilip Ganguly, Neeraj Rastogi, Ru-Jin Huang, Jaroslaw Necki, Junji Cao, Sachchida N. Tripathi, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 21, 717–730, https://doi.org/10.5194/acp-21-717-2021, https://doi.org/10.5194/acp-21-717-2021, 2021
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We present a simple conceptual framework based on elemental size distributions and enrichment factors that allows for a characterization of major sources, site-to-site similarities, and local differences and the identification of key information required for efficient policy development. Absolute concentrations are by far the highest in Delhi, followed by Beijing, and then the European cities.
Ivar R. van der Velde, Guido R. van der Werf, Sander Houweling, Henk J. Eskes, J. Pepijn Veefkind, Tobias Borsdorff, and Ilse Aben
Atmos. Chem. Phys., 21, 597–616, https://doi.org/10.5194/acp-21-597-2021, https://doi.org/10.5194/acp-21-597-2021, 2021
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This paper compares the relative atmospheric enhancements of CO and NO2 measured by the space-based instrument TROPOMI over different fire-prone ecosystems around the world. We find distinct spatial and temporal patterns in the ΔNO2 / ΔCO ratio that correspond to regional differences in combustion efficiency. This joint analysis provides a better understanding of regional-scale combustion characteristics and can help the fire modeling community to improve existing global emission inventories.
James L. France, Prudence Bateson, Pamela Dominutti, Grant Allen, Stephen Andrews, Stephane Bauguitte, Max Coleman, Tom Lachlan-Cope, Rebecca E. Fisher, Langwen Huang, Anna E. Jones, James Lee, David Lowry, Joseph Pitt, Ruth Purvis, John Pyle, Jacob Shaw, Nicola Warwick, Alexandra Weiss, Shona Wilde, Jonathan Witherstone, and Stuart Young
Atmos. Meas. Tech., 14, 71–88, https://doi.org/10.5194/amt-14-71-2021, https://doi.org/10.5194/amt-14-71-2021, 2021
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Measuring emission rates of methane from installations is tricky, and it is even more so when those installations are located offshore. Here, we show the aircraft set-up and demonstrate an effective methodology for surveying emissions from UK and Dutch offshore oil and gas installations. We present example data collected from two campaigns to demonstrate the challenges and solutions encountered during these surveys.
Gerrit Kuhlmann, Dominik Brunner, Grégoire Broquet, and Yasjka Meijer
Atmos. Meas. Tech., 13, 6733–6754, https://doi.org/10.5194/amt-13-6733-2020, https://doi.org/10.5194/amt-13-6733-2020, 2020
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The European CO2M mission is a proposed constellation of CO2 imaging satellites expected to monitor CO2 emissions of large cities. Using synthetic observations, we show that a constellation of two or more satellites should be able to quantify Berlin's annual emissions with 10–20 % accuracy, even when considering atmospheric transport model errors. We therefore expect that CO2M will make an important contribution to the monitoring and verification of CO2 emissions from cities worldwide.
Patrick A. Barker, Grant Allen, Martin Gallagher, Joseph R. Pitt, Rebecca E. Fisher, Thomas Bannan, Euan G. Nisbet, Stéphane J.-B. Bauguitte, Dominika Pasternak, Samuel Cliff, Marina B. Schimpf, Archit Mehra, Keith N. Bower, James D. Lee, Hugh Coe, and Carl J. Percival
Atmos. Chem. Phys., 20, 15443–15459, https://doi.org/10.5194/acp-20-15443-2020, https://doi.org/10.5194/acp-20-15443-2020, 2020
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Africa is estimated to account for approximately 52 % of global biomass burning (BB) carbon emissions. Despite this, there has been little previous in situ study of African BB emissions. This work presents BB emission factors for various atmospheric trace gases sampled from an aircraft in two distinct areas of Africa (Senegal and Uganda). Intracontinental variability in biomass burning methane emission is identified, which is attributed to difference in the specific fuel mixtures burnt.
Hossein Maazallahi, Julianne M. Fernandez, Malika Menoud, Daniel Zavala-Araiza, Zachary D. Weller, Stefan Schwietzke, Joseph C. von Fischer, Hugo Denier van der Gon, and Thomas Röckmann
Atmos. Chem. Phys., 20, 14717–14740, https://doi.org/10.5194/acp-20-14717-2020, https://doi.org/10.5194/acp-20-14717-2020, 2020
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Methane accounts for ∼ 25 % of current climate warming. The current lack of methane measurements is a barrier for tracking major sources, which are key for near-term climate mitigation. We use mobile measurements to identify and quantify methane emission sources in Utrecht (NL) and Hamburg (DE) with a focus on natural gas pipeline leaks. The measurements resulted in fixing the major leaks by the local utility, but coordinated efforts are needed at national levels for further emission reductions.
Bernhard Bereiter, Béla Tuzson, Philipp Scheidegger, André Kupferschmid, Herbert Looser, Lars Mächler, Daniel Baggenstos, Jochen Schmitt, Hubertus Fischer, and Lukas Emmenegger
Atmos. Meas. Tech., 13, 6391–6406, https://doi.org/10.5194/amt-13-6391-2020, https://doi.org/10.5194/amt-13-6391-2020, 2020
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The record of past greenhouse gas composition from ice cores is crucial for our understanding of global climate change. Deciphering this archive requires highly accurate and spatially resolved analysis of the very small amount of gas that is trapped in the ice. This is achieved with a mid-IR laser absorption spectrometer that provides simultaneous, high-precision measurements of CH4, N2O, CO2, and δ13C(CO2) and which will be coupled to a quantitative sublimation extraction method.
Joram J. D. Hooghiem, Maria Elena Popa, Thomas Röckmann, Jens-Uwe Grooß, Ines Tritscher, Rolf Müller, Rigel Kivi, and Huilin Chen
Atmos. Chem. Phys., 20, 13985–14003, https://doi.org/10.5194/acp-20-13985-2020, https://doi.org/10.5194/acp-20-13985-2020, 2020
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Wildfires release a large quantity of pollutants that can reach the stratosphere through pyro-convection events. In September 2017, a stratospheric plume was accidentally sampled during balloon soundings in northern Finland. The source of the plume was identified to be wildfire smoke based on in situ measurements of carbon monoxide (CO) and stable isotope analysis of CO. Furthermore, the age of the plume was estimated using backwards transport modelling to be ~24 d, with its origin in Canada.
Jinhwa Shin, Christoph Nehrbass-Ahles, Roberto Grilli, Jai Chowdhry Beeman, Frédéric Parrenin, Grégory Teste, Amaelle Landais, Loïc Schmidely, Lucas Silva, Jochen Schmitt, Bernhard Bereiter, Thomas F. Stocker, Hubertus Fischer, and Jérôme Chappellaz
Clim. Past, 16, 2203–2219, https://doi.org/10.5194/cp-16-2203-2020, https://doi.org/10.5194/cp-16-2203-2020, 2020
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We reconstruct atmospheric CO2 from the EPICA Dome C ice core during Marine Isotope Stage 6 (185–135 ka) to understand carbon mechanisms under the different boundary conditions of the climate system. The amplitude of CO2 is highly determined by the Northern Hemisphere stadial duration. Carbon dioxide maxima show different lags with respect to the corresponding abrupt CH4 jumps, the latter reflecting rapid warming in the Northern Hemisphere.
Stelios Myriokefalitakis, Nikos Daskalakis, Angelos Gkouvousis, Andreas Hilboll, Twan van Noije, Jason E. Williams, Philippe Le Sager, Vincent Huijnen, Sander Houweling, Tommi Bergman, Johann Rasmus Nüß, Mihalis Vrekoussis, Maria Kanakidou, and Maarten C. Krol
Geosci. Model Dev., 13, 5507–5548, https://doi.org/10.5194/gmd-13-5507-2020, https://doi.org/10.5194/gmd-13-5507-2020, 2020
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This work documents and evaluates the detailed tropospheric gas-phase chemical mechanism MOGUNTIA in the three-dimensional chemistry transport model TM5-MP. The Rosenbrock solver, as generated by the KPP software, is implemented in the chemistry code, which can successfully replace the classical Euler backward integration method. The MOGUNTIA scheme satisfactorily simulates a large suite of oxygenated volatile organic compounds (VOCs) that are observed in the atmosphere at significant levels.
Ying Zhu, Jia Chen, Xiao Bi, Gerrit Kuhlmann, Ka Lok Chan, Florian Dietrich, Dominik Brunner, Sheng Ye, and Mark Wenig
Atmos. Chem. Phys., 20, 13241–13251, https://doi.org/10.5194/acp-20-13241-2020, https://doi.org/10.5194/acp-20-13241-2020, 2020
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Average NO2 concentration of on-street mobile measurements (MMs) near the monitoring stations (MSs) was found to be considerably higher than the MSs data. The common measurement height (H) and distance (D) of the MSs result in 27 % lower average concentrations in total than the concentration of our MMs. Another 21 % difference remained after correcting the influence of the measuring H and D. This result makes our city-wide measurements for capturing the full range of concentrations necessary.
Alina Fiehn, Julian Kostinek, Maximilian Eckl, Theresa Klausner, Michał Gałkowski, Jinxuan Chen, Christoph Gerbig, Thomas Röckmann, Hossein Maazallahi, Martina Schmidt, Piotr Korbeń, Jarosław Neçki, Pawel Jagoda, Norman Wildmann, Christian Mallaun, Rostyslav Bun, Anna-Leah Nickl, Patrick Jöckel, Andreas Fix, and Anke Roiger
Atmos. Chem. Phys., 20, 12675–12695, https://doi.org/10.5194/acp-20-12675-2020, https://doi.org/10.5194/acp-20-12675-2020, 2020
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A severe reduction of greenhouse gas emissions is necessary to fulfill the Paris Agreement. We use aircraft- and ground-based in situ observations of trace gases and wind speed from two flights over the Upper Silesian Coal Basin, Poland, for independent emission estimation. The derived methane emission estimates are within the range of emission inventories, carbon dioxide estimates are in the lower range and carbon monoxide emission estimates are slightly higher than emission inventory values.
Jann Schrod, Dominik Kleinhenz, Maria Hörhold, Tobias Erhardt, Sarah Richter, Frank Wilhelms, Hubertus Fischer, Martin Ebert, Birthe Twarloh, Damiano Della Lunga, Camilla M. Jensen, Joachim Curtius, and Heinz G. Bingemer
Atmos. Chem. Phys., 20, 12459–12482, https://doi.org/10.5194/acp-20-12459-2020, https://doi.org/10.5194/acp-20-12459-2020, 2020
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Ice-nucleating particle (INP) concentrations of the last 6 centuries are presented from an ice core in Greenland. The data are accompanied by physical and chemical aerosol data. INPs are correlated to the dust signal from the ice core and seem to follow the annual input of mineral dust. We find no clear trend in the INP concentration. However, modern-day concentrations are higher and more variable than the concentrations of the past. This might have significant atmospheric implications.
Guillaume Monteil, Grégoire Broquet, Marko Scholze, Matthew Lang, Ute Karstens, Christoph Gerbig, Frank-Thomas Koch, Naomi E. Smith, Rona L. Thompson, Ingrid T. Luijkx, Emily White, Antoon Meesters, Philippe Ciais, Anita L. Ganesan, Alistair Manning, Michael Mischurow, Wouter Peters, Philippe Peylin, Jerôme Tarniewicz, Matt Rigby, Christian Rödenbeck, Alex Vermeulen, and Evie M. Walton
Atmos. Chem. Phys., 20, 12063–12091, https://doi.org/10.5194/acp-20-12063-2020, https://doi.org/10.5194/acp-20-12063-2020, 2020
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The paper presents the first results from the EUROCOM project, a regional atmospheric inversion intercomparison exercise involving six European research groups. It aims to produce an estimate of the net carbon flux between the European terrestrial ecosystems and the atmosphere for the period 2006–2015, based on constraints provided by observed CO2 concentrations and using inverse modelling techniques. The use of six different models enables us to investigate the robustness of the results.
Anna K. Tobler, Alicja Skiba, Dongyu S. Wang, Philip Croteau, Katarzyna Styszko, Jarosław Nęcki, Urs Baltensperger, Jay G. Slowik, and André S. H. Prévôt
Atmos. Meas. Tech., 13, 5293–5301, https://doi.org/10.5194/amt-13-5293-2020, https://doi.org/10.5194/amt-13-5293-2020, 2020
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Some quadrupole aerosol chemical speciation monitors (Q-ACSMs) have had issues with the quantification of particulate chloride, resulting in apparent negative chloride concentrations. We can show that this is due to the different behavior of Cl+ and HCl+, and we present a correction for the more accurate quantification of chloride. The correction can be applied to measurements in environments where the particulate chloride is dominated by NH4Cl.
Béla Tuzson, Manuel Graf, Jonas Ravelid, Philipp Scheidegger, André Kupferschmid, Herbert Looser, Randulph Paulo Morales, and Lukas Emmenegger
Atmos. Meas. Tech., 13, 4715–4726, https://doi.org/10.5194/amt-13-4715-2020, https://doi.org/10.5194/amt-13-4715-2020, 2020
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We describe a lightweight (2 kg) mid-IR laser spectrometer for airborne, in situ atmospheric methane (CH4) measurements. The instrument, based on an open-path circular multipass cell, provides fast response (1 Hz) and sub-parts-per-billion precision. It can easily be mounted on a drone, giving access to highly resolved 4D (spatial and temporal) data. The performance was assessed during field deployments involving artificial CH4 releases and vertical concentration gradients in the PBL.
Srijana Lama, Sander Houweling, K. Folkert Boersma, Henk Eskes, Ilse Aben, Hugo A. C. Denier van der Gon, Maarten C. Krol, Han Dolman, Tobias Borsdorff, and Alba Lorente
Atmos. Chem. Phys., 20, 10295–10310, https://doi.org/10.5194/acp-20-10295-2020, https://doi.org/10.5194/acp-20-10295-2020, 2020
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Rapid urbanization has increased the consumption of fossil fuel, contributing the degradation of urban air quality. Burning efficiency is a major factor determining the impact of fuel burning on the environment. We quantify the burning efficiency of fossil fuel use over six megacities using satellite remote sensing data. City governance can use these results to understand air pollution scenarios and to formulate effective air pollution control strategies.
Jordi Vilà-Guerau de Arellano, Patrizia Ney, Oscar Hartogensis, Hugo de Boer, Kevin van Diepen, Dzhaner Emin, Geiske de Groot, Anne Klosterhalfen, Matthias Langensiepen, Maria Matveeva, Gabriela Miranda-García, Arnold F. Moene, Uwe Rascher, Thomas Röckmann, Getachew Adnew, Nicolas Brüggemann, Youri Rothfuss, and Alexander Graf
Biogeosciences, 17, 4375–4404, https://doi.org/10.5194/bg-17-4375-2020, https://doi.org/10.5194/bg-17-4375-2020, 2020
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The CloudRoots field experiment has obtained an open comprehensive observational data set that includes soil, plant, and atmospheric variables to investigate the interactions between a heterogeneous land surface and its overlying atmospheric boundary layer, including the rapid perturbations of clouds in evapotranspiration. Our findings demonstrate that in order to understand and represent diurnal variability, we need to measure and model processes from the leaf to the landscape scales.
Johannes C. Laube, Emma C. Leedham Elvidge, Karina E. Adcock, Bianca Baier, Carl A. M. Brenninkmeijer, Huilin Chen, Elise S. Droste, Jens-Uwe Grooß, Pauli Heikkinen, Andrew J. Hind, Rigel Kivi, Alexander Lojko, Stephen A. Montzka, David E. Oram, Steve Randall, Thomas Röckmann, William T. Sturges, Colm Sweeney, Max Thomas, Elinor Tuffnell, and Felix Ploeger
Atmos. Chem. Phys., 20, 9771–9782, https://doi.org/10.5194/acp-20-9771-2020, https://doi.org/10.5194/acp-20-9771-2020, 2020
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We demonstrate that AirCore technology, which is based on small low-cost balloons, can provide access to trace gas measurements such as CFCs at ultra-low abundances. This is a new way to quantify ozone-depleting, and related, substances in the stratosphere, which is largely inaccessible to aircraft. We show two potential uses: (a) tracking the stratospheric circulation, which is predicted to change, and (b) assessing three common meteorological reanalyses driving a global stratospheric model.
Anders Svensson, Dorthe Dahl-Jensen, Jørgen Peder Steffensen, Thomas Blunier, Sune O. Rasmussen, Bo M. Vinther, Paul Vallelonga, Emilie Capron, Vasileios Gkinis, Eliza Cook, Helle Astrid Kjær, Raimund Muscheler, Sepp Kipfstuhl, Frank Wilhelms, Thomas F. Stocker, Hubertus Fischer, Florian Adolphi, Tobias Erhardt, Michael Sigl, Amaelle Landais, Frédéric Parrenin, Christo Buizert, Joseph R. McConnell, Mirko Severi, Robert Mulvaney, and Matthias Bigler
Clim. Past, 16, 1565–1580, https://doi.org/10.5194/cp-16-1565-2020, https://doi.org/10.5194/cp-16-1565-2020, 2020
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We identify signatures of large bipolar volcanic eruptions in Greenland and Antarctic ice cores during the last glacial period, which allows for a precise temporal alignment of the ice cores. Thereby the exact timing of unexplained, abrupt climatic changes occurring during the last glacial period can be determined in a global context. The study thus provides a step towards a full understanding of elements of the climate system that may also play an important role in the future.
Marc Schwaerzel, Claudia Emde, Dominik Brunner, Randulph Morales, Thomas Wagner, Alexis Berne, Brigitte Buchmann, and Gerrit Kuhlmann
Atmos. Meas. Tech., 13, 4277–4293, https://doi.org/10.5194/amt-13-4277-2020, https://doi.org/10.5194/amt-13-4277-2020, 2020
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Horizontal homogeneity is often assumed for trace gases remote sensing, although it is not valid where trace gas concentrations have high spatial variability, e.g., in cities. We show the importance of 3D effects for MAX-DOAS and airborne imaging spectrometers using 3D-box air mass factors implemented in the MYSTIC radiative transfer solver. In both cases, 3D information is invaluable for interpreting the measurements, as not considering 3D effects can lead to misinterpretation of measurements.
Getachew Agmuas Adnew, Thijs L. Pons, Gerbrand Koren, Wouter Peters, and Thomas Röckmann
Biogeosciences, 17, 3903–3922, https://doi.org/10.5194/bg-17-3903-2020, https://doi.org/10.5194/bg-17-3903-2020, 2020
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We measured the effect of photosynthesis, the largest flux in the carbon cycle, on the triple oxygen isotope composition of atmospheric CO2 at the leaf level during gas exchange using three plant species. The main factors that limit the impact of land vegetation on the triple oxygen isotope composition of atmospheric CO2 are identified, characterized and discussed. The effect of photosynthesis on the isotopic composition of CO2 is commonly quantified as discrimination (ΔA).
Marielle Saunois, Ann R. Stavert, Ben Poulter, Philippe Bousquet, Josep G. Canadell, Robert B. Jackson, Peter A. Raymond, Edward J. Dlugokencky, Sander Houweling, Prabir K. Patra, Philippe Ciais, Vivek K. Arora, David Bastviken, Peter Bergamaschi, Donald R. Blake, Gordon Brailsford, Lori Bruhwiler, Kimberly M. Carlson, Mark Carrol, Simona Castaldi, Naveen Chandra, Cyril Crevoisier, Patrick M. Crill, Kristofer Covey, Charles L. Curry, Giuseppe Etiope, Christian Frankenberg, Nicola Gedney, Michaela I. Hegglin, Lena Höglund-Isaksson, Gustaf Hugelius, Misa Ishizawa, Akihiko Ito, Greet Janssens-Maenhout, Katherine M. Jensen, Fortunat Joos, Thomas Kleinen, Paul B. Krummel, Ray L. Langenfelds, Goulven G. Laruelle, Licheng Liu, Toshinobu Machida, Shamil Maksyutov, Kyle C. McDonald, Joe McNorton, Paul A. Miller, Joe R. Melton, Isamu Morino, Jurek Müller, Fabiola Murguia-Flores, Vaishali Naik, Yosuke Niwa, Sergio Noce, Simon O'Doherty, Robert J. Parker, Changhui Peng, Shushi Peng, Glen P. Peters, Catherine Prigent, Ronald Prinn, Michel Ramonet, Pierre Regnier, William J. Riley, Judith A. Rosentreter, Arjo Segers, Isobel J. Simpson, Hao Shi, Steven J. Smith, L. Paul Steele, Brett F. Thornton, Hanqin Tian, Yasunori Tohjima, Francesco N. Tubiello, Aki Tsuruta, Nicolas Viovy, Apostolos Voulgarakis, Thomas S. Weber, Michiel van Weele, Guido R. van der Werf, Ray F. Weiss, Doug Worthy, Debra Wunch, Yi Yin, Yukio Yoshida, Wenxin Zhang, Zhen Zhang, Yuanhong Zhao, Bo Zheng, Qing Zhu, Qiuan Zhu, and Qianlai Zhuang
Earth Syst. Sci. Data, 12, 1561–1623, https://doi.org/10.5194/essd-12-1561-2020, https://doi.org/10.5194/essd-12-1561-2020, 2020
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Understanding and quantifying the global methane (CH4) budget is important for assessing realistic pathways to mitigate climate change. We have established a consortium of multidisciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate new research aimed at improving and regularly updating the global methane budget. This is the second version of the review dedicated to the decadal methane budget, integrating results of top-down and bottom-up estimates.
Michael Müller, Peter Graf, Jonas Meyer, Anastasia Pentina, Dominik Brunner, Fernando Perez-Cruz, Christoph Hüglin, and Lukas Emmenegger
Atmos. Meas. Tech., 13, 3815–3834, https://doi.org/10.5194/amt-13-3815-2020, https://doi.org/10.5194/amt-13-3815-2020, 2020
Fortunat Joos, Renato Spahni, Benjamin D. Stocker, Sebastian Lienert, Jurek Müller, Hubertus Fischer, Jochen Schmitt, I. Colin Prentice, Bette Otto-Bliesner, and Zhengyu Liu
Biogeosciences, 17, 3511–3543, https://doi.org/10.5194/bg-17-3511-2020, https://doi.org/10.5194/bg-17-3511-2020, 2020
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Results of the first globally resolved simulations of terrestrial carbon and nitrogen (N) cycling and N2O emissions over the past 21 000 years are compared with reconstructed N2O emissions. Modelled and reconstructed emissions increased strongly during past abrupt warming events. This evidence appears consistent with a dynamic response of biological N fixation to increasing N demand by ecosystems, thereby reducing N limitation of plant productivity and supporting a land sink for atmospheric CO2.
Longfei Yu, Eliza Harris, Stephan Henne, Sarah Eggleston, Martin Steinbacher, Lukas Emmenegger, Christoph Zellweger, and Joachim Mohn
Atmos. Chem. Phys., 20, 6495–6519, https://doi.org/10.5194/acp-20-6495-2020, https://doi.org/10.5194/acp-20-6495-2020, 2020
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We observed the isotopic composition of nitrous oxide in the unpolluted air at Jungfraujoch for 5 years. Our results indicate a clear seasonal pattern in the isotopic composition, corresponding with that in atmospheric nitrous oxide levels. This is most likely due to temporal variations in both emission processes and air mass sources for Jungfraujoch. Our findings are of importance to global nitrous oxide modelling and to better understanding of long-term trends in atmospheric nitrous oxide.
Stephen J. Harris, Jesper Liisberg, Longlong Xia, Jing Wei, Kerstin Zeyer, Longfei Yu, Matti Barthel, Benjamin Wolf, Bryce F. J. Kelly, Dioni I. Cendón, Thomas Blunier, Johan Six, and Joachim Mohn
Atmos. Meas. Tech., 13, 2797–2831, https://doi.org/10.5194/amt-13-2797-2020, https://doi.org/10.5194/amt-13-2797-2020, 2020
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The latest commercial laser spectrometers have the potential to revolutionize N2O isotope analysis. However, to do so, they must be able to produce trustworthy data. Here, we test the performance of widely used laser spectrometers for ambient air applications and identify instrument-specific dependencies on gas matrix and trace gas concentrations. We then provide a calibration workflow to facilitate the operation of these instruments in order to generate reproducible and accurate data.
Michael Jähn, Gerrit Kuhlmann, Qing Mu, Jean-Matthieu Haussaire, David Ochsner, Katherine Osterried, Valentin Clément, and Dominik Brunner
Geosci. Model Dev., 13, 2379–2392, https://doi.org/10.5194/gmd-13-2379-2020, https://doi.org/10.5194/gmd-13-2379-2020, 2020
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Emission inventories of air pollutants and greenhouse gases are widely used as input for atmospheric chemistry transport models. However, the pre-processing of these data is both time-consuming and requires a large amount of disk storage. To overcome this issue, a Python package has been developed and tested for two different models. There, the inventory is projected to the model grid and scaling factors are provided. This approach saves computational time while remaining numerically equivalent.
Peter H. Zimmermann, Carl A. M. Brenninkmeijer, Andrea Pozzer, Patrick Jöckel, Franziska Winterstein, Andreas Zahn, Sander Houweling, and Jos Lelieveld
Atmos. Chem. Phys., 20, 5787–5809, https://doi.org/10.5194/acp-20-5787-2020, https://doi.org/10.5194/acp-20-5787-2020, 2020
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The atmospheric abundance of the greenhouse gas methane is determined by interacting emission sources and sinks in a dynamic global environment. In this study, its global budget from 1997 to 2016 is simulated with a general circulation model using emission estimates of 11 source categories. The model results are evaluated against 17 ground station and 320 intercontinental flight observation series. Deviations are used to re-scale the emission quantities with the aim of matching observations.
Stuart K. Grange, Hanspeter Lötscher, Andrea Fischer, Lukas Emmenegger, and Christoph Hueglin
Atmos. Meas. Tech., 13, 1867–1885, https://doi.org/10.5194/amt-13-1867-2020, https://doi.org/10.5194/amt-13-1867-2020, 2020
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Black carbon (BC) is an important atmospheric pollutant and can be monitored by instruments called aethalometers. A pragmatic data processing technique called the
aethalometer modelcan be used to apportion aethalometer observations into traffic and woodburning components. We present an exploratory data analysis evaluating the aethalometer model and use the outputs for BC trend analysis across Switzerland. The aethalometer model's robustness and utility for such analyses is discussed.
Gianluca Mussetti, Dominik Brunner, Stephan Henne, Jonas Allegrini, E. Scott Krayenhoff, Sebastian Schubert, Christian Feigenwinter, Roland Vogt, Andreas Wicki, and Jan Carmeliet
Geosci. Model Dev., 13, 1685–1710, https://doi.org/10.5194/gmd-13-1685-2020, https://doi.org/10.5194/gmd-13-1685-2020, 2020
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Street trees are regarded as a powerful measure to reduce excessive heat in cities. To enable city-wide studies of the cooling effect of street trees, we developed a coupled urban climate model with explicit representation of street trees (COSMO-BEP-Tree). The model compares well with surface, flux and satellite observations and responds realistically to changes in tree characteristics. Street trees largely impact energy fluxes and wind speed, while air temperatures are only slightly reduced.
Jia Chen, Florian Dietrich, Hossein Maazallahi, Andreas Forstmaier, Dominik Winkler, Magdalena E. G. Hofmann, Hugo Denier van der Gon, and Thomas Röckmann
Atmos. Chem. Phys., 20, 3683–3696, https://doi.org/10.5194/acp-20-3683-2020, https://doi.org/10.5194/acp-20-3683-2020, 2020
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We demonstrate for the first time that large festivals can be significant methane sources, though they are not included in emission inventories. We combined in situ measurements with a Gaussian plume model to determine the Oktoberfest emissions and show that they are not due solely to human biogenic emissions, but are instead primarily fossil fuel related. Our study provides the foundation to develop reduction policies for such events and new pathways to mitigate fossil fuel methane emissions.
Stefan Lossow, Charlotta Högberg, Farahnaz Khosrawi, Gabriele P. Stiller, Ralf Bauer, Kaley A. Walker, Sylvia Kellmann, Andrea Linden, Michael Kiefer, Norbert Glatthor, Thomas von Clarmann, Donal P. Murtagh, Jörg Steinwagner, Thomas Röckmann, and Roland Eichinger
Atmos. Meas. Tech., 13, 287–308, https://doi.org/10.5194/amt-13-287-2020, https://doi.org/10.5194/amt-13-287-2020, 2020
Gerrit Kuhlmann, Grégoire Broquet, Julia Marshall, Valentin Clément, Armin Löscher, Yasjka Meijer, and Dominik Brunner
Atmos. Meas. Tech., 12, 6695–6719, https://doi.org/10.5194/amt-12-6695-2019, https://doi.org/10.5194/amt-12-6695-2019, 2019
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The Copernicus Anthropogenic CO2 Monitoring (CO2M) mission is a proposed constellation of imaging satellites with a CO2 instrument as main payload and optionally instruments for NO2, CO and aerosols. This study demonstrates the huge benefit of an NO2 instrument for detecting city plumes and weak point sources. Its main advantages are the higher signal-to-noise ratio and the lower sensitivity to clouds that significantly increases the number of observations available for quantifying CO2 emission.
Marco de Bruine, Maarten Krol, Jordi Vilà-Guerau de Arellano, and Thomas Röckmann
Geosci. Model Dev., 12, 5177–5196, https://doi.org/10.5194/gmd-12-5177-2019, https://doi.org/10.5194/gmd-12-5177-2019, 2019
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An aerosol scheme with multiple aerosol species is introduced in the Dutch Atmospheric Large-Eddy Simulation model (DALES) and focused to simulate the feedback of aerosol–cloud interaction (ACI) on the aerosol population. Cloud aerosol processing is found to be sensitive to the numerical method, while removal by precipitation is more stable. How ACI increases or decreases the mean aerosol size depends on the balance between the evaporation of clouds/rain and ultimate removal by precipitation.
Ignacio Pisso, Espen Sollum, Henrik Grythe, Nina I. Kristiansen, Massimo Cassiani, Sabine Eckhardt, Delia Arnold, Don Morton, Rona L. Thompson, Christine D. Groot Zwaaftink, Nikolaos Evangeliou, Harald Sodemann, Leopold Haimberger, Stephan Henne, Dominik Brunner, John F. Burkhart, Anne Fouilloux, Jerome Brioude, Anne Philipp, Petra Seibert, and Andreas Stohl
Geosci. Model Dev., 12, 4955–4997, https://doi.org/10.5194/gmd-12-4955-2019, https://doi.org/10.5194/gmd-12-4955-2019, 2019
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We present the latest release of the Lagrangian transport model FLEXPART, which simulates the transport, diffusion, dry and wet deposition, radioactive decay, and 1st-order chemical reactions of atmospheric tracers. The model has been recently updated both technically and in the representation of physicochemical processes. We describe the changes, document the most recent input and output files, provide working examples, and introduce testing capabilities.
Christoph Zellweger, Rainer Steinbrecher, Olivier Laurent, Haeyoung Lee, Sumin Kim, Lukas Emmenegger, Martin Steinbacher, and Brigitte Buchmann
Atmos. Meas. Tech., 12, 5863–5878, https://doi.org/10.5194/amt-12-5863-2019, https://doi.org/10.5194/amt-12-5863-2019, 2019
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We analysed results obtained through CO and N2O performance audits conducted within the framework of the Global Atmosphere Watch (GAW) quality management system of the World Meteorology Organization (WMO). The results reveal that current spectroscopic measurement techniques have clear advantages with respect to data quality objectives compared to more traditional methods. Further, they allow for a smooth continuation of historic CO and N2O time series.
Łukasz Chmura, Michał Gałkowski, Piotr Sekuła, Mirosław Zimnoch, Jarosław Nęcki, Jakub Bartyzel, Damian Zięba, Kazimierz Różański, Wojciech Wołkowicz, and Laszlo Haszpra
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2019-748, https://doi.org/10.5194/acp-2019-748, 2019
Revised manuscript not accepted
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The rise of temperatures across the globe, mainly attributed to the anthropogenic emissions of greenhouse gases, is predicted to have an increased impact on ecosystems over the next century. One of the manifestations of this anthropogenic global warming will be the increased occurrence of prolonged droughts in the temperate climate zones. In the current study we present the evidence of an increased impact of droughts on the annual cycle of carbon dioxide over Central-Eastern Europe.
Hubertus Fischer, Jochen Schmitt, Michael Bock, Barbara Seth, Fortunat Joos, Renato Spahni, Sebastian Lienert, Gianna Battaglia, Benjamin D. Stocker, Adrian Schilt, and Edward J. Brook
Biogeosciences, 16, 3997–4021, https://doi.org/10.5194/bg-16-3997-2019, https://doi.org/10.5194/bg-16-3997-2019, 2019
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N2O concentrations were subject to strong variations accompanying glacial–interglacial but also rapid climate changes over the last 21 kyr. The sources of these N2O changes can be identified by measuring the isotopic composition of N2O in ice cores and using the distinct isotopic composition of terrestrial and marine N2O. We show that both marine and terrestrial sources increased from the last glacial to the Holocene but that only terrestrial emissions responded quickly to rapid climate changes.
Andreas Luther, Ralph Kleinschek, Leon Scheidweiler, Sara Defratyka, Mila Stanisavljevic, Andreas Forstmaier, Alexandru Dandocsi, Sebastian Wolff, Darko Dubravica, Norman Wildmann, Julian Kostinek, Patrick Jöckel, Anna-Leah Nickl, Theresa Klausner, Frank Hase, Matthias Frey, Jia Chen, Florian Dietrich, Jarosław Nȩcki, Justyna Swolkień, Andreas Fix, Anke Roiger, and André Butz
Atmos. Meas. Tech., 12, 5217–5230, https://doi.org/10.5194/amt-12-5217-2019, https://doi.org/10.5194/amt-12-5217-2019, 2019
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Methane ventilated from hard coal mines in the Upper Silesian
Coal Basin in Poland is measured with a mobile Fourier transform spectrometer EM27/SUN. The instrument was mounted on a truck driving in stop-and-go patterns downwind of the methane sources. The emissions are estimated with the cross-sectional flux method. Calculated emissions are in broad agreement with the E-PRTR database. Wind-related errors on the methane estimates dominate the error budget and typically amount to 20 %.
Erkan Ibraim, Benjamin Wolf, Eliza Harris, Rainer Gasche, Jing Wei, Longfei Yu, Ralf Kiese, Sarah Eggleston, Klaus Butterbach-Bahl, Matthias Zeeman, Béla Tuzson, Lukas Emmenegger, Johan Six, Stephan Henne, and Joachim Mohn
Biogeosciences, 16, 3247–3266, https://doi.org/10.5194/bg-16-3247-2019, https://doi.org/10.5194/bg-16-3247-2019, 2019
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Nitrous oxide (N2O) is an important greenhouse gas and the major stratospheric ozone-depleting substance; therefore, mitigation of anthropogenic N2O emissions is needed. To trace N2O-emitting source processes, in this study, we observed N2O isotopocules above an intensively managed grassland research site with a recently developed laser spectroscopy method. Our results indicate that the domain of denitrification or nitrifier denitrification was the major N2O source.
Stuart N. Riddick, Denise L. Mauzerall, Michael Celia, Neil R. P. Harris, Grant Allen, Joseph Pitt, John Staunton-Sykes, Grant L. Forster, Mary Kang, David Lowry, Euan G. Nisbet, and Alistair J. Manning
Atmos. Chem. Phys., 19, 9787–9796, https://doi.org/10.5194/acp-19-9787-2019, https://doi.org/10.5194/acp-19-9787-2019, 2019
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Currently, bottom-up methods estimate that 0.13 % of methane produced by UK North Sea oil and gas installations is lost. Here we measure emissions from eight platforms in the North Sea and, when considered collectively, the methane loss is estimated at 0.19 % of gas production. As this ambient loss is not explicitly accounted for in the bottom-up approach, these measured emissions represent significant additional emissions above previous estimates.
Johannes Sutter, Hubertus Fischer, Klaus Grosfeld, Nanna B. Karlsson, Thomas Kleiner, Brice Van Liefferinge, and Olaf Eisen
The Cryosphere, 13, 2023–2041, https://doi.org/10.5194/tc-13-2023-2019, https://doi.org/10.5194/tc-13-2023-2019, 2019
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The Antarctic Ice Sheet may have played an important role in moderating the transition between warm and cold climate epochs over the last million years. We find that the Antarctic Ice Sheet grew considerably about 0.9 Myr ago, a time when ice-age–warm-age cycles changed from a
40 000 to a 100 000 year periodicity. Our findings also suggest that ice as old as 1.5 Myr still exists at the bottom of the East Antarctic Ice Sheet despite the major climate reorganisations in the past.
Tobias Erhardt, Emilie Capron, Sune Olander Rasmussen, Simon Schüpbach, Matthias Bigler, Florian Adolphi, and Hubertus Fischer
Clim. Past, 15, 811–825, https://doi.org/10.5194/cp-15-811-2019, https://doi.org/10.5194/cp-15-811-2019, 2019
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The cause of the rapid warming events documented in proxy records across the Northern Hemisphere during the last glacial has been a long-standing puzzle in paleo-climate research. Here, we use high-resolution ice-core data from to cores in Greenland to investigate the progression during the onset of these events on multi-annual timescales to test their plausible triggers. We show that atmospheric circulation changes preceded the warming in Greenland and the collapse of the sea ice by a decade.
Dominik Brunner, Gerrit Kuhlmann, Julia Marshall, Valentin Clément, Oliver Fuhrer, Grégoire Broquet, Armin Löscher, and Yasjka Meijer
Atmos. Chem. Phys., 19, 4541–4559, https://doi.org/10.5194/acp-19-4541-2019, https://doi.org/10.5194/acp-19-4541-2019, 2019
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Atmospheric transport models are increasingly being used to estimate CO2 emissions from atmospheric CO2 measurements. This study demonstrates the importance of distributing CO2 emissions vertically in the model according to realistic profiles, since a major proportion of CO2 is emitted through tall stacks from power plants and industrial sources. With the traditional approach of emitting all CO2 at the surface, models may significantly overestimate the atmospheric CO2 levels.
Tobias Borsdorff, Joost aan de Brugh, Sudhanshu Pandey, Otto Hasekamp, Ilse Aben, Sander Houweling, and Jochen Landgraf
Atmos. Chem. Phys., 19, 3579–3588, https://doi.org/10.5194/acp-19-3579-2019, https://doi.org/10.5194/acp-19-3579-2019, 2019
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The Tropospheric Monitoring Instrument (TROPOMI) on the Sentinel-5 Precursor satellite provides carbon monoxide (CO) total column concentrations based on measurements in the 2.3 μm spectral range with a spatial resolution of 7 km x 7 km and daily global coverage. In this study, we analyzed local CO enhancements in an area around Iran from 1 November to 20 December 2017 using the WRF model and evaluated CO emissions from the cities of Tehran, Yerevan, Urmia, and Tabriz.
Iris N. Dekker, Sander Houweling, Sudhanshu Pandey, Maarten Krol, Thomas Röckmann, Tobias Borsdorff, Jochen Landgraf, and Ilse Aben
Atmos. Chem. Phys., 19, 3433–3445, https://doi.org/10.5194/acp-19-3433-2019, https://doi.org/10.5194/acp-19-3433-2019, 2019
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During November 2017, very high pollution levels were measured in the northern part of India. In this study, satellite (TROPOMI) data and model (WRF) data on carbon monoxide (CO) are studied to investigate the main sources of the CO pollution over the Indo-Gangetic Plain. We found that residential and commercial combustion was a much more important source of CO than the post-monsoon crop burning during this period. Meteorology was found important in the accumulation and ventilation of CO.
Dušan Materić, Elke Ludewig, Kangming Xu, Thomas Röckmann, and Rupert Holzinger
The Cryosphere, 13, 297–307, https://doi.org/10.5194/tc-13-297-2019, https://doi.org/10.5194/tc-13-297-2019, 2019
Stephen M. Platt, Sabine Eckhardt, Benedicte Ferré, Rebecca E. Fisher, Ove Hermansen, Pär Jansson, David Lowry, Euan G. Nisbet, Ignacio Pisso, Norbert Schmidbauer, Anna Silyakova, Andreas Stohl, Tove M. Svendby, Sunil Vadakkepuliyambatta, Jürgen Mienert, and Cathrine Lund Myhre
Atmos. Chem. Phys., 18, 17207–17224, https://doi.org/10.5194/acp-18-17207-2018, https://doi.org/10.5194/acp-18-17207-2018, 2018
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We measured atmospheric mixing ratios of methane over the Arctic Ocean around Svalbard and compared observed variations to inventories for anthropogenic, wetland, and biomass burning methane emissions and an atmospheric transport model. With knowledge of where variations were expected due to the aforementioned land-based emissions, we were able to identify and quantify a methane source from the ocean north of Svalbard, likely from sub-sea hydrocarbon seeps and/or gas hydrate decomposition.
Jonas Beck, Michael Bock, Jochen Schmitt, Barbara Seth, Thomas Blunier, and Hubertus Fischer
Biogeosciences, 15, 7155–7175, https://doi.org/10.5194/bg-15-7155-2018, https://doi.org/10.5194/bg-15-7155-2018, 2018
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Ice core concentration and stable isotope measurements of atmospheric CH4 give valuable insights into the CH4 cycle of the past. New carbon and hydrogen stable isotope CH4 data measured on ice from both Greenland and Antarctica over the Holocene allow us to draw conclusions on the methane emission processes. In particular, our results cast doubt on a hypothesis proposing early human land use to be responsible for the atmospheric methane concentration increase in the second half of the Holocene.
Florian Adolphi, Christopher Bronk Ramsey, Tobias Erhardt, R. Lawrence Edwards, Hai Cheng, Chris S. M. Turney, Alan Cooper, Anders Svensson, Sune O. Rasmussen, Hubertus Fischer, and Raimund Muscheler
Clim. Past, 14, 1755–1781, https://doi.org/10.5194/cp-14-1755-2018, https://doi.org/10.5194/cp-14-1755-2018, 2018
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The last glacial period was characterized by a number of rapid climate changes seen, for example, as abrupt warmings in Greenland and changes in monsoon rainfall intensity. However, due to chronological uncertainties it is challenging to know how tightly coupled these changes were. Here we exploit cosmogenic signals caused by changes in the Sun and Earth magnetic fields to link different climate archives and improve our understanding of the dynamics of abrupt climate change.
Rocío Baró, Pedro Jiménez-Guerrero, Martin Stengel, Dominik Brunner, Gabriele Curci, Renate Forkel, Lucy Neal, Laura Palacios-Peña, Nicholas Savage, Martijn Schaap, Paolo Tuccella, Hugo Denier van der Gon, and Stefano Galmarini
Atmos. Chem. Phys., 18, 15183–15199, https://doi.org/10.5194/acp-18-15183-2018, https://doi.org/10.5194/acp-18-15183-2018, 2018
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Particles in the atmosphere, such as pollution, desert dust, and volcanic ash, have an impact on meteorology. They interact with incoming radiation resulting in a cooling effect of the atmosphere. Today, the use of meteorology and chemistry models help us to understand these processes, but there are a lot of uncertainties. The goal of this work is to evaluate how these interactions are represented in the models by comparing them to satellite data to see how close they are to reality.
Sandy P. Harrison, Patrick J. Bartlein, Victor Brovkin, Sander Houweling, Silvia Kloster, and I. Colin Prentice
Earth Syst. Dynam., 9, 663–677, https://doi.org/10.5194/esd-9-663-2018, https://doi.org/10.5194/esd-9-663-2018, 2018
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Temperature affects fire occurrence and severity. Warming will increase fire-related carbon emissions and thus atmospheric CO2. The size of this feedback is not known. We use charcoal records to estimate pre-industrial fire emissions and a simple land–biosphere model to quantify the feedback. We infer a feedback strength of 5.6 3.2 ppm CO2 per degree of warming and a gain of 0.09 ± 0.05 for a climate sensitivity of 2.8 K. Thus, fire feedback is a large part of the climate–carbon-cycle feedback.
P. Morten Hundt, Michael Müller, Markus Mangold, Béla Tuzson, Philipp Scheidegger, Herbert Looser, Christoph Hüglin, and Lukas Emmenegger
Atmos. Meas. Tech., 11, 2669–2681, https://doi.org/10.5194/amt-11-2669-2018, https://doi.org/10.5194/amt-11-2669-2018, 2018
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NO2 is a pollutant that regularly exceeds its limit values in European cities. We developed a compact, mobile laser spectrometer that measures NO2 concentrations and installed it on a tram in Zurich. Mobile operation resulted in NO2 concentration data with high spatio-temporal resolution. The data were validated against fixed air-quality monitoring sites and provided detailed insights into the spatio-temporal concentration distribution of NO2 in an urban environment.
Marco de Bruine, Maarten Krol, Twan van Noije, Philippe Le Sager, and Thomas Röckmann
Geosci. Model Dev., 11, 1443–1465, https://doi.org/10.5194/gmd-11-1443-2018, https://doi.org/10.5194/gmd-11-1443-2018, 2018
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Precipitation evaporation (PE) and subsequent aerosol resuspension (AR) are currently ignored or implemented only crudely in GCMs. This research introduces PE to Earth system model EC-Earth and explores ways to treat AR and the impact on global aerosol burden. Simple 1:1 scaling of AR with PE leads to an increase (+8 to 15.9 %). Taking into account raindrop size distribution and/or accounting for in-rain aerosol processing decreases aerosol burden -1.5 to 6.2 % and -10 to -11 %, respectively.
Laura Palacios-Peña, Rocío Baró, Alexander Baklanov, Alessandra Balzarini, Dominik Brunner, Renate Forkel, Marcus Hirtl, Luka Honzak, José María López-Romero, Juan Pedro Montávez, Juan Luis Pérez, Guido Pirovano, Roberto San José, Wolfram Schröder, Johannes Werhahn, Ralf Wolke, Rahela Žabkar, and Pedro Jiménez-Guerrero
Atmos. Chem. Phys., 18, 5021–5043, https://doi.org/10.5194/acp-18-5021-2018, https://doi.org/10.5194/acp-18-5021-2018, 2018
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Atmospheric aerosols modify the radiative budget of the Earth, and it is therefore mandatory to have an accurate representation of their optical properties for understanding their climatic role. This work therefore evaluates the skill in the representation of optical properties by different remote-sensing sensors and regional online coupled chemistry–climate models over Europe.
Karina E. Adcock, Claire E. Reeves, Lauren J. Gooch, Emma C. Leedham Elvidge, Matthew J. Ashfold, Carl A. M. Brenninkmeijer, Charles Chou, Paul J. Fraser, Ray L. Langenfelds, Norfazrin Mohd Hanif, Simon O'Doherty, David E. Oram, Chang-Feng Ou-Yang, Siew Moi Phang, Azizan Abu Samah, Thomas Röckmann, William T. Sturges, and Johannes C. Laube
Atmos. Chem. Phys., 18, 4737–4751, https://doi.org/10.5194/acp-18-4737-2018, https://doi.org/10.5194/acp-18-4737-2018, 2018
James D. Lee, Stephen D. Mobbs, Axel Wellpott, Grant Allen, Stephane J.-B. Bauguitte, Ralph R. Burton, Richard Camilli, Hugh Coe, Rebecca E. Fisher, James L. France, Martin Gallagher, James R. Hopkins, Mathias Lanoiselle, Alastair C. Lewis, David Lowry, Euan G. Nisbet, Ruth M. Purvis, Sebastian O'Shea, John A. Pyle, and Thomas B. Ryerson
Atmos. Meas. Tech., 11, 1725–1739, https://doi.org/10.5194/amt-11-1725-2018, https://doi.org/10.5194/amt-11-1725-2018, 2018
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This work describes measurements, made from an aircraft platform, of the emission of methane and other organic gases from an uncontrolled leak from an oil platform in the North Sea (Total Elgin). The measurements made helped the platform operators to devise a strategy for repairing the leak and serve as a methodology for assessing future similar incidents.
Fabian Schoenenberger, Stephan Henne, Matthias Hill, Martin K. Vollmer, Giorgos Kouvarakis, Nikolaos Mihalopoulos, Simon O'Doherty, Michela Maione, Lukas Emmenegger, Thomas Peter, and Stefan Reimann
Atmos. Chem. Phys., 18, 4069–4092, https://doi.org/10.5194/acp-18-4069-2018, https://doi.org/10.5194/acp-18-4069-2018, 2018
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Anthropogenic halocarbon emissions contribute to stratospheric ozone depletion and global warming. We measured atmospheric halocarbons for 6 months on Crete to extend the coverage of the existing observation network to the Eastern Mediterranean. The derived emission estimates showed a contribution of 16.8 % (13.6–23.3 %) and 53.2 % (38.1–84.2 %) of this region to the total HFC and HCFC emissions of the analyzed European domain and a reduction of the underlying uncertainties by 40–80 %.
Abdelhadi El Yazidi, Michel Ramonet, Philippe Ciais, Gregoire Broquet, Isabelle Pison, Amara Abbaris, Dominik Brunner, Sebastien Conil, Marc Delmotte, Francois Gheusi, Frederic Guerin, Lynn Hazan, Nesrine Kachroudi, Giorgos Kouvarakis, Nikolaos Mihalopoulos, Leonard Rivier, and Dominique Serça
Atmos. Meas. Tech., 11, 1599–1614, https://doi.org/10.5194/amt-11-1599-2018, https://doi.org/10.5194/amt-11-1599-2018, 2018
Masa Kageyama, Pascale Braconnot, Sandy P. Harrison, Alan M. Haywood, Johann H. Jungclaus, Bette L. Otto-Bliesner, Jean-Yves Peterschmitt, Ayako Abe-Ouchi, Samuel Albani, Patrick J. Bartlein, Chris Brierley, Michel Crucifix, Aisling Dolan, Laura Fernandez-Donado, Hubertus Fischer, Peter O. Hopcroft, Ruza F. Ivanovic, Fabrice Lambert, Daniel J. Lunt, Natalie M. Mahowald, W. Richard Peltier, Steven J. Phipps, Didier M. Roche, Gavin A. Schmidt, Lev Tarasov, Paul J. Valdes, Qiong Zhang, and Tianjun Zhou
Geosci. Model Dev., 11, 1033–1057, https://doi.org/10.5194/gmd-11-1033-2018, https://doi.org/10.5194/gmd-11-1033-2018, 2018
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The Paleoclimate Modelling Intercomparison Project (PMIP) takes advantage of the existence of past climate states radically different from the recent past to test climate models used for climate projections and to better understand these climates. This paper describes the PMIP contribution to CMIP6 (Coupled Model Intercomparison Project, 6th phase) and possible analyses based on PMIP results, as well as on other CMIP6 projects.
Emma C. Leedham Elvidge, Harald Bönisch, Carl A. M. Brenninkmeijer, Andreas Engel, Paul J. Fraser, Eileen Gallacher, Ray Langenfelds, Jens Mühle, David E. Oram, Eric A. Ray, Anna R. Ridley, Thomas Röckmann, William T. Sturges, Ray F. Weiss, and Johannes C. Laube
Atmos. Chem. Phys., 18, 3369–3385, https://doi.org/10.5194/acp-18-3369-2018, https://doi.org/10.5194/acp-18-3369-2018, 2018
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Chemical species measured in stratospheric air can be used as proxies for stratospheric circulation changes which cannot be measured directly. A range of tracers is important to understand changing stratospheric dynamics. We demonstrate the suitability of PFCs and HFCs as tracers and support recent work that reduces the current stratospheric lifetime of SF6. Updates to policy-relevant parameters (e.g. stratospheric lifetime) linked to this change are provided for O3-depleting substances.
Taku Umezawa, Carl A. M. Brenninkmeijer, Thomas Röckmann, Carina van der Veen, Stanley C. Tyler, Ryo Fujita, Shinji Morimoto, Shuji Aoki, Todd Sowers, Jochen Schmitt, Michael Bock, Jonas Beck, Hubertus Fischer, Sylvia E. Michel, Bruce H. Vaughn, John B. Miller, James W. C. White, Gordon Brailsford, Hinrich Schaefer, Peter Sperlich, Willi A. Brand, Michael Rothe, Thomas Blunier, David Lowry, Rebecca E. Fisher, Euan G. Nisbet, Andrew L. Rice, Peter Bergamaschi, Cordelia Veidt, and Ingeborg Levin
Atmos. Meas. Tech., 11, 1207–1231, https://doi.org/10.5194/amt-11-1207-2018, https://doi.org/10.5194/amt-11-1207-2018, 2018
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Isotope measurements are useful for separating different methane sources. However, the lack of widely accepted standards and calibration methods for stable carbon and hydrogen isotopic ratios of methane in air has caused significant measurement offsets among laboratories. We conducted worldwide interlaboratory comparisons, surveyed the literature and assessed them systematically. This study may be of help in future attempts to harmonize data sets of isotopic composition of atmospheric methane.
Peter Bergamaschi, Ute Karstens, Alistair J. Manning, Marielle Saunois, Aki Tsuruta, Antoine Berchet, Alexander T. Vermeulen, Tim Arnold, Greet Janssens-Maenhout, Samuel Hammer, Ingeborg Levin, Martina Schmidt, Michel Ramonet, Morgan Lopez, Jost Lavric, Tuula Aalto, Huilin Chen, Dietrich G. Feist, Christoph Gerbig, László Haszpra, Ove Hermansen, Giovanni Manca, John Moncrieff, Frank Meinhardt, Jaroslaw Necki, Michal Galkowski, Simon O'Doherty, Nina Paramonova, Hubertus A. Scheeren, Martin Steinbacher, and Ed Dlugokencky
Atmos. Chem. Phys., 18, 901–920, https://doi.org/10.5194/acp-18-901-2018, https://doi.org/10.5194/acp-18-901-2018, 2018
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European methane (CH4) emissions are estimated for 2006–2012 using atmospheric in situ measurements from 18 European monitoring stations and 7 different inverse models. Our analysis highlights the potential significant contribution of natural emissions from wetlands (including peatlands and wet soils) to the total European emissions. The top-down estimates of total EU-28 CH4 emissions are broadly consistent with the sum of reported anthropogenic CH4 emissions and the estimated natural emissions.
Pascal Bohleber, Tobias Erhardt, Nicole Spaulding, Helene Hoffmann, Hubertus Fischer, and Paul Mayewski
Clim. Past, 14, 21–37, https://doi.org/10.5194/cp-14-21-2018, https://doi.org/10.5194/cp-14-21-2018, 2018
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The Colle Gnifetti (CG) glacier is the only drilling site in the European Alps offering ice core records back to some 1000 years. We aim to fully exploit these unique long-term records by establishing a reliable long-term age scale and an improved ice core proxy interpretation for reconstructing temperature. Our findings reveal a site-specific temperature-related signal in the trends of the mineral dust proxy Ca2+ that may supplement other proxy evidence over the last millennium.
Iris N. Dekker, Sander Houweling, Ilse Aben, Thomas Röckmann, Maarten Krol, Sara Martínez-Alonso, Merritt N. Deeter, and Helen M. Worden
Atmos. Chem. Phys., 17, 14675–14694, https://doi.org/10.5194/acp-17-14675-2017, https://doi.org/10.5194/acp-17-14675-2017, 2017
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This study estimates carbon monoxide emissions from the city of Madrid using MOPITT satellite data. There are two methods used and reviewed in this paper: a method that can only estimate a trend in the emission and a newly developed method that also includes model data from WRF to quantify the emissions. We find Madrid CO emissions to be lower by 48 % for 2002 and by 17 % for 2006 compared with the EdgarV4.2 emission inventory, but uncertainty (20 to 50 %) remains.
Yu Liu, Nicolas Gruber, and Dominik Brunner
Atmos. Chem. Phys., 17, 14145–14169, https://doi.org/10.5194/acp-17-14145-2017, https://doi.org/10.5194/acp-17-14145-2017, 2017
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We analyze fossil fuel signals in atmospheric CO2 over Europe using a high-resolution atmospheric transport model and diurnal emission data. We find that fossil fuel CO2 accounts for more than half of the atmospheric CO2 variations, mainly at diurnal timescales. The covariance of diurnal emission and transport also leads to a substantial rectification effect. Thus, the consideration of diurnal emissions and high-resolution transport is paramount for accurately modeling the fossil fuel signal.
Bette L. Otto-Bliesner, Pascale Braconnot, Sandy P. Harrison, Daniel J. Lunt, Ayako Abe-Ouchi, Samuel Albani, Patrick J. Bartlein, Emilie Capron, Anders E. Carlson, Andrea Dutton, Hubertus Fischer, Heiko Goelzer, Aline Govin, Alan Haywood, Fortunat Joos, Allegra N. LeGrande, William H. Lipscomb, Gerrit Lohmann, Natalie Mahowald, Christoph Nehrbass-Ahles, Francesco S. R. Pausata, Jean-Yves Peterschmitt, Steven J. Phipps, Hans Renssen, and Qiong Zhang
Geosci. Model Dev., 10, 3979–4003, https://doi.org/10.5194/gmd-10-3979-2017, https://doi.org/10.5194/gmd-10-3979-2017, 2017
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The PMIP4 and CMIP6 mid-Holocene and Last Interglacial simulations provide an opportunity to examine the impact of two different changes in insolation forcing on climate at times when other forcings were relatively similar to present. This will allow exploration of the role of feedbacks relevant to future projections. Evaluating these simulations using paleoenvironmental data will provide direct out-of-sample tests of the reliability of state-of-the-art models to simulate climate changes.
Frédéric Parrenin, Marie G. P. Cavitte, Donald D. Blankenship, Jérôme Chappellaz, Hubertus Fischer, Olivier Gagliardini, Valérie Masson-Delmotte, Olivier Passalacqua, Catherine Ritz, Jason Roberts, Martin J. Siegert, and Duncan A. Young
The Cryosphere, 11, 2427–2437, https://doi.org/10.5194/tc-11-2427-2017, https://doi.org/10.5194/tc-11-2427-2017, 2017
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The oldest dated deep ice core drilled in Antarctica has been retrieved at EPICA Dome C (EDC), reaching ~ 800 000 years. Obtaining an older palaeoclimatic record from Antarctica is one of the greatest challenges of the ice core community. Here, we estimate the age of basal ice in the Dome C area. We find that old ice (> 1.5 Myr) likely exists in two regions a few tens of kilometres away from EDC:
Little Dome C Patchand
North Patch.
Marielle Saunois, Philippe Bousquet, Ben Poulter, Anna Peregon, Philippe Ciais, Josep G. Canadell, Edward J. Dlugokencky, Giuseppe Etiope, David Bastviken, Sander Houweling, Greet Janssens-Maenhout, Francesco N. Tubiello, Simona Castaldi, Robert B. Jackson, Mihai Alexe, Vivek K. Arora, David J. Beerling, Peter Bergamaschi, Donald R. Blake, Gordon Brailsford, Lori Bruhwiler, Cyril Crevoisier, Patrick Crill, Kristofer Covey, Christian Frankenberg, Nicola Gedney, Lena Höglund-Isaksson, Misa Ishizawa, Akihiko Ito, Fortunat Joos, Heon-Sook Kim, Thomas Kleinen, Paul Krummel, Jean-François Lamarque, Ray Langenfelds, Robin Locatelli, Toshinobu Machida, Shamil Maksyutov, Joe R. Melton, Isamu Morino, Vaishali Naik, Simon O'Doherty, Frans-Jan W. Parmentier, Prabir K. Patra, Changhui Peng, Shushi Peng, Glen P. Peters, Isabelle Pison, Ronald Prinn, Michel Ramonet, William J. Riley, Makoto Saito, Monia Santini, Ronny Schroeder, Isobel J. Simpson, Renato Spahni, Atsushi Takizawa, Brett F. Thornton, Hanqin Tian, Yasunori Tohjima, Nicolas Viovy, Apostolos Voulgarakis, Ray Weiss, David J. Wilton, Andy Wiltshire, Doug Worthy, Debra Wunch, Xiyan Xu, Yukio Yoshida, Bowen Zhang, Zhen Zhang, and Qiuan Zhu
Atmos. Chem. Phys., 17, 11135–11161, https://doi.org/10.5194/acp-17-11135-2017, https://doi.org/10.5194/acp-17-11135-2017, 2017
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Following the Global Methane Budget 2000–2012 published in Saunois et al. (2016), we use the same dataset of bottom-up and top-down approaches to discuss the variations in methane emissions over the period 2000–2012. The changes in emissions are discussed both in terms of trends and quasi-decadal changes. The ensemble gathered here allows us to synthesise the robust changes in terms of regional and sectorial contributions to the increasing methane emissions.
Antoine Berchet, Katrin Zink, Dietmar Oettl, Jürg Brunner, Lukas Emmenegger, and Dominik Brunner
Geosci. Model Dev., 10, 3441–3459, https://doi.org/10.5194/gmd-10-3441-2017, https://doi.org/10.5194/gmd-10-3441-2017, 2017
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We evaluate a new cost-effective method to simulate pollutant dispersion at high resolution on a city-wide domain. The method is based on a catalogue of reference simulations matched to weather observations to produce a sequence of hourly pollution maps. A total of 2 years of simulations are compared with continuous measurements and passive NO2 samplers in the city of Zurich. Spatial and temporal variability proved to be very well reproduced by the method.
Johan Martinsson, Guillaume Monteil, Moa K. Sporre, Anne Maria Kaldal Hansen, Adam Kristensson, Kristina Eriksson Stenström, Erik Swietlicki, and Marianne Glasius
Atmos. Chem. Phys., 17, 11025–11040, https://doi.org/10.5194/acp-17-11025-2017, https://doi.org/10.5194/acp-17-11025-2017, 2017
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This study attempts to link observations of biogenic organic compounds found in atmospheric particles to landscape exposure of the incoming air mass. The results revealed that several of the observed compounds were connected to exposure of coniferous forests. There were also a number of landscape types that did not contribute to the biogenic organic compounds, sea and ocean as an example. This type of methodology may be important in order to study land use changes impact on air quality.
Tesfaye A. Berhanu, Sönke Szidat, Dominik Brunner, Ece Satar, Rüdiger Schanda, Peter Nyfeler, Michael Battaglia, Martin Steinbacher, Samuel Hammer, and Markus Leuenberger
Atmos. Chem. Phys., 17, 10753–10766, https://doi.org/10.5194/acp-17-10753-2017, https://doi.org/10.5194/acp-17-10753-2017, 2017
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Fossil fuel CO2 is the major contributor of anthropogenic CO2 in the atmosphere, and accurate quantification is essential to better understand the carbon cycle. Such accurate quantification can be conducted based on radiocarbon measurements. In this study, we present radiocarbon measurements from a tall tower site in Switzerland. From these measurements, we have observed seasonally varying fossil fuel CO2 contributions and a biospheric CO2 component that varies diurnally and seasonally.
Dominik Brunner, Tim Arnold, Stephan Henne, Alistair Manning, Rona L. Thompson, Michela Maione, Simon O'Doherty, and Stefan Reimann
Atmos. Chem. Phys., 17, 10651–10674, https://doi.org/10.5194/acp-17-10651-2017, https://doi.org/10.5194/acp-17-10651-2017, 2017
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Hydrofluorocarbons (HFCs) and SF6 are industrially produced gases with a large greenhouse-gas warming potential. In this study, we estimated the emissions of HFCs and SF6 over Europe by combining measurements at three background stations with four different model systems. We identified significant differences between our estimates and nationally reported numbers, but also found that the network of only three sites in Europe is insufficient to reliably attribute emissions to individual countries.
Eleni Athanasopoulou, Orestis Speyer, Dominik Brunner, Heike Vogel, Bernhard Vogel, Nikolaos Mihalopoulos, and Evangelos Gerasopoulos
Atmos. Chem. Phys., 17, 10597–10618, https://doi.org/10.5194/acp-17-10597-2017, https://doi.org/10.5194/acp-17-10597-2017, 2017
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This work focuses on the impact of residential wood burning on aerosol levels, composition and radiation under the ongoing economic crisis in Greece. The atmospheric model COSMO-ART performed a series of runs during the winter of 2013–2014. Emission inputs were revised according to the detailed aerosol characterization by local measurements. Aerosol levels were found to be elevated and mostly composed of organics, yet the timing of the plume justifies the minor radiative cooling and feedbacks.
Yann Poltera, Giovanni Martucci, Martine Collaud Coen, Maxime Hervo, Lukas Emmenegger, Stephan Henne, Dominik Brunner, and Alexander Haefele
Atmos. Chem. Phys., 17, 10051–10070, https://doi.org/10.5194/acp-17-10051-2017, https://doi.org/10.5194/acp-17-10051-2017, 2017
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We present the PathfinderTURB algorithm for the analysis of ceilometer backscatter data and the real-time detection of the vertical structure of the planetary boundary layer. PathfinderTURB has been applied to 1 year of data measured by two ceilometers operated at two Swiss stations: the Aerological Observatory of Payerne on the Swiss plateau, and the Alpine Jungfraujoch observatory. The study shows that aerosols from the boundary layer significantly influence the air measured at Jungfraujoch.
Rocío Baró, Laura Palacios-Peña, Alexander Baklanov, Alessandra Balzarini, Dominik Brunner, Renate Forkel, Marcus Hirtl, Luka Honzak, Juan Luis Pérez, Guido Pirovano, Roberto San José, Wolfram Schröder, Johannes Werhahn, Ralf Wolke, Rahela Žabkar, and Pedro Jiménez-Guerrero
Atmos. Chem. Phys., 17, 9677–9696, https://doi.org/10.5194/acp-17-9677-2017, https://doi.org/10.5194/acp-17-9677-2017, 2017
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The influence on modeled max., mean and min. temperature over Europe of including aerosol–radiation–cloud interactions has been assessed for two case studies in 2010. Data were taken from an ensemble of online regional chemistry–climate models from EuMetChem COST Action. The results indicate that including these interactions clearly improves the spatiotemporal variability in the temperature signal simulated by the models, with implications for reducing the uncertainty in climate projections.
Stuart N. Riddick, Sarah Connors, Andrew D. Robinson, Alistair J. Manning, Pippa S. D. Jones, David Lowry, Euan Nisbet, Robert L. Skelton, Grant Allen, Joseph Pitt, and Neil R. P. Harris
Atmos. Chem. Phys., 17, 7839–7851, https://doi.org/10.5194/acp-17-7839-2017, https://doi.org/10.5194/acp-17-7839-2017, 2017
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High methane mixing ratios occurred at our long-term measurement site. Isotopic measurements show the source is a landfill 7 km away; the emissions were estimated using three different approaches. The emission estimates made by near-source and middle-distance methods agree well for a period of intense observation. The estimate of the inverse modelling is similar to the labour-intensive middle-distance approach, which shows it can be used to identify point sources within an emission landscape.
Peter Köhler, Christoph Nehrbass-Ahles, Jochen Schmitt, Thomas F. Stocker, and Hubertus Fischer
Earth Syst. Sci. Data, 9, 363–387, https://doi.org/10.5194/essd-9-363-2017, https://doi.org/10.5194/essd-9-363-2017, 2017
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We document our best available data compilation of published ice core records of the greenhouse gases CO2, CH4, and N2O and recent measurements on firn air and atmospheric samples covering the time window from 156 000 years BP to the beginning of the year 2016 CE. A smoothing spline method is applied to translate the discrete and irregularly spaced data points into continuous time series. The radiative forcing for each greenhouse gas is computed using well-established, simple formulations.
Julien G. Anet, Martin Steinbacher, Laura Gallardo, Patricio A. Velásquez Álvarez, Lukas Emmenegger, and Brigitte Buchmann
Atmos. Chem. Phys., 17, 6477–6492, https://doi.org/10.5194/acp-17-6477-2017, https://doi.org/10.5194/acp-17-6477-2017, 2017
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There are less long-term surface ozone measurements on the Southern than on the Northern Hemisphere, which makes it difficult to thoroughly understand global ozone chemistry. We have analyzed a new, 20-year-long ozone dataset measured at 2200 m asl at El Tololo, Chile, and show that the annual cycle of ozone is mainly driven by ozone transport from the stratosphere to the troposphere. As well, we illustrate that the timing of the annual maximum is regressing to earlier in the year.
Carl Meusinger, Ulrike Dusek, Stephanie M. King, Rupert Holzinger, Thomas Rosenørn, Peter Sperlich, Maxime Julien, Gerald S. Remaud, Merete Bilde, Thomas Röckmann, and Matthew S. Johnson
Atmos. Chem. Phys., 17, 6373–6391, https://doi.org/10.5194/acp-17-6373-2017, https://doi.org/10.5194/acp-17-6373-2017, 2017
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Isotope studies can constrain budgets of secondary organic aerosol (SOA) that is pivotal to air pollution and climate. SOA from α-pinene ozonolysis was found to be enriched in 13C relative to the precursor. The observed difference in 13C between the gas and particle phases may arise from isotope-dependent changes in branching ratios. Alternatively, some gas-phase products involve carbon atoms from highly enriched and depleted sites, giving a non-kinetic origin to the observed fractionations.
Célia J. Sapart, Natalia Shakhova, Igor Semiletov, Joachim Jansen, Sönke Szidat, Denis Kosmach, Oleg Dudarev, Carina van der Veen, Matthias Egger, Valentine Sergienko, Anatoly Salyuk, Vladimir Tumskoy, Jean-Louis Tison, and Thomas Röckmann
Biogeosciences, 14, 2283–2292, https://doi.org/10.5194/bg-14-2283-2017, https://doi.org/10.5194/bg-14-2283-2017, 2017
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The Arctic Ocean, especially the Siberian shelves, overlays large areas of subsea permafrost that is degrading. We show that methane with a biogenic origin is emitted from this permafrost. At locations where bubble plumes have been observed, methane can escape oxidation in the surface sediment and rapidly migrate through the very shallow water column of this region to escape to the atmosphere, generating a positive radiative feedback.
Markella Prokopiou, Patricia Martinerie, Célia J. Sapart, Emmanuel Witrant, Guillaume Monteil, Kentaro Ishijima, Sophie Bernard, Jan Kaiser, Ingeborg Levin, Thomas Blunier, David Etheridge, Ed Dlugokencky, Roderik S. W. van de Wal, and Thomas Röckmann
Atmos. Chem. Phys., 17, 4539–4564, https://doi.org/10.5194/acp-17-4539-2017, https://doi.org/10.5194/acp-17-4539-2017, 2017
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Nitrous oxide is the third most important anthropogenic greenhouse gas with an increasing mole fraction. To understand its natural and anthropogenic sources
we employ isotope measurements. Results show that while the N2O mole fraction increases, its heavy isotope content decreases. The isotopic changes observed underline the dominance of agricultural emissions especially at the early part of the record, whereas in the later decades the contribution from other anthropogenic sources increases.
Aki Tsuruta, Tuula Aalto, Leif Backman, Janne Hakkarainen, Ingrid T. van der Laan-Luijkx, Maarten C. Krol, Renato Spahni, Sander Houweling, Marko Laine, Ed Dlugokencky, Angel J. Gomez-Pelaez, Marcel van der Schoot, Ray Langenfelds, Raymond Ellul, Jgor Arduini, Francesco Apadula, Christoph Gerbig, Dietrich G. Feist, Rigel Kivi, Yukio Yoshida, and Wouter Peters
Geosci. Model Dev., 10, 1261–1289, https://doi.org/10.5194/gmd-10-1261-2017, https://doi.org/10.5194/gmd-10-1261-2017, 2017
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In this study, we found that the average global methane emission for 2000–2012, estimated by the CTE-CH4 model, was 516±51 Tg CH4 yr-1, and the estimates for 2007–2012 were 4 % larger than for 2000–2006. The model estimates are sensitive to inputs and setups, but according to sensitivity tests the study suggests that the increase in atmospheric methane concentrations during 21st century was due to an increase in emissions from the 35S-EQ latitudinal bands.
Ulrike Dusek, Regina Hitzenberger, Anne Kasper-Giebl, Magdalena Kistler, Harro A. J. Meijer, Sönke Szidat, Lukas Wacker, Rupert Holzinger, and Thomas Röckmann
Atmos. Chem. Phys., 17, 3233–3251, https://doi.org/10.5194/acp-17-3233-2017, https://doi.org/10.5194/acp-17-3233-2017, 2017
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Measurements of the radioactive carbon isotope 14C allow to identify the sources of aerosol carbon. We report an extensive 14C source apportionment record in the Netherlands with samples covering a whole year. We discovered that long-range transport has a large influence on aerosol carbon levels. Fossil fuel carbon is least influenced by long-range transport and more regional in origin. Biomass burning seems to be a minor source of aerosol carbon in the Netherlands.
Laura Palacios-Peña, Rocío Baró, Juan Luis Guerrero-Rascado, Lucas Alados-Arboledas, Dominik Brunner, and Pedro Jiménez-Guerrero
Atmos. Chem. Phys., 17, 277–296, https://doi.org/10.5194/acp-17-277-2017, https://doi.org/10.5194/acp-17-277-2017, 2017
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The effects of atmospheric aerosols over the Earth’s climate mainly depend on their optical, microphysical and chemical properties, which modify the Earth's radiative budget, the main source of uncertainty in climate change. In this work we have studied the representation of aerosol optical properties using an online coupled model (WRF-Chem) when aerosol–radiation interactions (ARIs) and aerosol–clouds interactions (ACIs) are taken into account over the Iberian Peninsula.
Sander Houweling, Peter Bergamaschi, Frederic Chevallier, Martin Heimann, Thomas Kaminski, Maarten Krol, Anna M. Michalak, and Prabir Patra
Atmos. Chem. Phys., 17, 235–256, https://doi.org/10.5194/acp-17-235-2017, https://doi.org/10.5194/acp-17-235-2017, 2017
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The aim of this paper is to present an overview of inverse modeling methods, developed over the years, for estimating the global sources and sinks of the greenhouse gas methane from atmospheric measurements. It provides insight into how techniques and estimates have evolved over time, what the remaining shortcomings are, new developments, and promising future directions.
Ioannis Kioutsioukis, Ulas Im, Efisio Solazzo, Roberto Bianconi, Alba Badia, Alessandra Balzarini, Rocío Baró, Roberto Bellasio, Dominik Brunner, Charles Chemel, Gabriele Curci, Hugo Denier van der Gon, Johannes Flemming, Renate Forkel, Lea Giordano, Pedro Jiménez-Guerrero, Marcus Hirtl, Oriol Jorba, Astrid Manders-Groot, Lucy Neal, Juan L. Pérez, Guidio Pirovano, Roberto San Jose, Nicholas Savage, Wolfram Schroder, Ranjeet S. Sokhi, Dimiter Syrakov, Paolo Tuccella, Johannes Werhahn, Ralf Wolke, Christian Hogrefe, and Stefano Galmarini
Atmos. Chem. Phys., 16, 15629–15652, https://doi.org/10.5194/acp-16-15629-2016, https://doi.org/10.5194/acp-16-15629-2016, 2016
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Four ensemble methods are applied to two annual AQMEII datasets and their performance is compared for O3, NO2 and PM10. The goal of the study is to quantify to what extent we can extract predictable signals from an ensemble with superior skill at each station over the single models and the ensemble mean. The promotion of the right amount of accuracy and diversity within the ensemble results in an average additional skill of up to 31 % compared to using the full ensemble in an unconditional way.
Bastiaan Jonkheid, Thomas Röckmann, Norbert Glatthor, Christof Janssen, Gabriele Stiller, and Thomas von Clarmann
Atmos. Meas. Tech., 9, 6069–6079, https://doi.org/10.5194/amt-9-6069-2016, https://doi.org/10.5194/amt-9-6069-2016, 2016
Marielle Saunois, Philippe Bousquet, Ben Poulter, Anna Peregon, Philippe Ciais, Josep G. Canadell, Edward J. Dlugokencky, Giuseppe Etiope, David Bastviken, Sander Houweling, Greet Janssens-Maenhout, Francesco N. Tubiello, Simona Castaldi, Robert B. Jackson, Mihai Alexe, Vivek K. Arora, David J. Beerling, Peter Bergamaschi, Donald R. Blake, Gordon Brailsford, Victor Brovkin, Lori Bruhwiler, Cyril Crevoisier, Patrick Crill, Kristofer Covey, Charles Curry, Christian Frankenberg, Nicola Gedney, Lena Höglund-Isaksson, Misa Ishizawa, Akihiko Ito, Fortunat Joos, Heon-Sook Kim, Thomas Kleinen, Paul Krummel, Jean-François Lamarque, Ray Langenfelds, Robin Locatelli, Toshinobu Machida, Shamil Maksyutov, Kyle C. McDonald, Julia Marshall, Joe R. Melton, Isamu Morino, Vaishali Naik, Simon O'Doherty, Frans-Jan W. Parmentier, Prabir K. Patra, Changhui Peng, Shushi Peng, Glen P. Peters, Isabelle Pison, Catherine Prigent, Ronald Prinn, Michel Ramonet, William J. Riley, Makoto Saito, Monia Santini, Ronny Schroeder, Isobel J. Simpson, Renato Spahni, Paul Steele, Atsushi Takizawa, Brett F. Thornton, Hanqin Tian, Yasunori Tohjima, Nicolas Viovy, Apostolos Voulgarakis, Michiel van Weele, Guido R. van der Werf, Ray Weiss, Christine Wiedinmyer, David J. Wilton, Andy Wiltshire, Doug Worthy, Debra Wunch, Xiyan Xu, Yukio Yoshida, Bowen Zhang, Zhen Zhang, and Qiuan Zhu
Earth Syst. Sci. Data, 8, 697–751, https://doi.org/10.5194/essd-8-697-2016, https://doi.org/10.5194/essd-8-697-2016, 2016
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An accurate assessment of the methane budget is important to understand the atmospheric methane concentrations and trends and to provide realistic pathways for climate change mitigation. The various and diffuse sources of methane as well and its oxidation by a very short lifetime radical challenge this assessment. We quantify the methane sources and sinks as well as their uncertainties based on both bottom-up and top-down approaches provided by a broad international scientific community.
Nicola J. Warwick, Michelle L. Cain, Rebecca Fisher, James L. France, David Lowry, Sylvia E. Michel, Euan G. Nisbet, Bruce H. Vaughn, James W. C. White, and John A. Pyle
Atmos. Chem. Phys., 16, 14891–14908, https://doi.org/10.5194/acp-16-14891-2016, https://doi.org/10.5194/acp-16-14891-2016, 2016
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Methane is an important greenhouse gas. Methane emissions from Arctic wetlands are poorly quantified and may increase in a warming climate. Using a global atmospheric model and atmospheric observations of methane and its isotopologues, we find that isotopologue data are useful in constraining Arctic wetland emissions. Our results suggest that the seasonal cycle of these emissions may be incorrectly simulated in land process models, with implications for our understanding of future emissions.
Dorota Janina Mrozek, Carina van der Veen, Magdalena E. G. Hofmann, Huilin Chen, Rigel Kivi, Pauli Heikkinen, and Thomas Röckmann
Atmos. Meas. Tech., 9, 5607–5620, https://doi.org/10.5194/amt-9-5607-2016, https://doi.org/10.5194/amt-9-5607-2016, 2016
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Stratospheric Air Sub-sampler (SAS) is a device to collect and to store the stratospheric profile of air collected with an AirCore (Karion et al., 2010) in numerous sub-samples. The sub-samples (each of 25 mL at ambient temperature and pressure) can be later introduced to the continuous flow systems to measure for example the isotopic composition of CO2. The performance of the coupled system is demonstrated for a set of air samples from an AirCore flight in November 2014 near Sodankylä, Finland.
Beatriz Sayuri Oyama, Maria de Fátima Andrade, Pierre Herckes, Ulrike Dusek, Thomas Röckmann, and Rupert Holzinger
Atmos. Chem. Phys., 16, 14397–14408, https://doi.org/10.5194/acp-16-14397-2016, https://doi.org/10.5194/acp-16-14397-2016, 2016
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Vehicular emissions have a strong impact on air pollution in big cities; hence, the study was performed in São Paulo city, where light- (LDVs) and heavy-duty vehicles (HDVs) run on different fuels. We find that organic aerosol emission from LDVs and HDVs is a complex process involving oxidation of fuel constituents, NOx chemistry, and condensation of unburned fuel hydrocarbons on new or existing particles. The obtained emission patterns can be used to study processing of young aerosol in Brazil.
Giulia Zazzeri, Dave Lowry, Rebecca E. Fisher, James L. France, Mathias Lanoisellé, Bryce F. J. Kelly, Jaroslaw M. Necki, Charlotte P. Iverach, Elisa Ginty, Miroslaw Zimnoch, Alina Jasek, and Euan G. Nisbet
Atmos. Chem. Phys., 16, 13669–13680, https://doi.org/10.5194/acp-16-13669-2016, https://doi.org/10.5194/acp-16-13669-2016, 2016
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Methane emissions estimates from the coal sector are highly uncertain. Precise δ13C isotopic signatures of methane sources can be used in atmospheric models for a methane budget assessment. Emissions from both underground and opencast coal mines in the UK, Australia and Poland were sampled and isotopically characterised using high-precision measurements of δ13C values. Representative isotopic signatures were provided, taking into account specific ranks of coal and mine type.
Michel Legrand, Joseph McConnell, Hubertus Fischer, Eric W. Wolff, Susanne Preunkert, Monica Arienzo, Nathan Chellman, Daiana Leuenberger, Olivia Maselli, Philip Place, Michael Sigl, Simon Schüpbach, and Mike Flannigan
Clim. Past, 12, 2033–2059, https://doi.org/10.5194/cp-12-2033-2016, https://doi.org/10.5194/cp-12-2033-2016, 2016
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Here, we review previous attempts made to reconstruct past forest fire using chemical signals recorded in Greenland ice. We showed that the Greenland ice records of ammonium, found to be a good fire proxy, consistently indicate changing fire activity in Canada in response to past climatic conditions that occurred since the last 15 000 years, including the Little Ice Age and the last large climatic transition.
Bette L. Otto-Bliesner, Pascale Braconnot, Sandy P. Harrison, Daniel J. Lunt, Ayako Abe-Ouchi, Samuel Albani, Patrick J. Bartlein, Emilie Capron, Anders E. Carlson, Andrea Dutton, Hubertus Fischer, Heiko Goelzer, Aline Govin, Alan Haywood, Fortunat Joos, Allegra N. Legrande, William H. Lipscomb, Gerrit Lohmann, Natalie Mahowald, Christoph Nehrbass-Ahles, Jean-Yves Peterschmidt, Francesco S.-R. Pausata, Steven Phipps, and Hans Renssen
Clim. Past Discuss., https://doi.org/10.5194/cp-2016-106, https://doi.org/10.5194/cp-2016-106, 2016
Preprint retracted
Olivier Eicher, Matthias Baumgartner, Adrian Schilt, Jochen Schmitt, Jakob Schwander, Thomas F. Stocker, and Hubertus Fischer
Clim. Past, 12, 1979–1993, https://doi.org/10.5194/cp-12-1979-2016, https://doi.org/10.5194/cp-12-1979-2016, 2016
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A new high-resolution total air content record over the NGRIP ice core, spanning 0.3–120 kyr is presented. In agreement with Antarctic ice cores, we find a strong local insolation signature but also 3–5 % decreases in total air content as a local response to Dansgaard–Oeschger events, which can only partly be explained by changes in surface pressure and temperature. Accordingly, a dynamic response of firnification to rapid climate changes on the Greenland ice sheet must have occurred.
Jochen Landgraf, Joost aan de Brugh, Remco Scheepmaker, Tobias Borsdorff, Haili Hu, Sander Houweling, Andre Butz, Ilse Aben, and Otto Hasekamp
Atmos. Meas. Tech., 9, 4955–4975, https://doi.org/10.5194/amt-9-4955-2016, https://doi.org/10.5194/amt-9-4955-2016, 2016
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In 2016, the Sentinel 5 Precursor mission will be launched, with the TROPOMI instrument as its single payload. It will deliver daily global measurements of carbon monoxide for air quality monitoring as part of the Copernicus atmospheric services. In this paper, we focus on the operational data processing of the CO product from TROPOMI measurements of the shortwave infrared spectral range, and we discuss the algorithm's maturity.
Amaelle Landais, Valérie Masson-Delmotte, Emilie Capron, Petra M. Langebroek, Pepijn Bakker, Emma J. Stone, Niklaus Merz, Christoph C. Raible, Hubertus Fischer, Anaïs Orsi, Frédéric Prié, Bo Vinther, and Dorthe Dahl-Jensen
Clim. Past, 12, 1933–1948, https://doi.org/10.5194/cp-12-1933-2016, https://doi.org/10.5194/cp-12-1933-2016, 2016
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The last lnterglacial (LIG; 116 000 to 129 000 years before present) surface temperature at the upstream Greenland NEEM deposition site is estimated to be warmer by +7 to +11 °C compared to the preindustrial period. We show that under such warm temperatures, melting of snow probably led to a significant surface melting. There is a paradox between the extent of the Greenland ice sheet during the LIG and the strong warming during this period that models cannot solve.
Andreas Ostler, Ralf Sussmann, Prabir K. Patra, Sander Houweling, Marko De Bruine, Gabriele P. Stiller, Florian J. Haenel, Johannes Plieninger, Philippe Bousquet, Yi Yin, Marielle Saunois, Kaley A. Walker, Nicholas M. Deutscher, David W. T. Griffith, Thomas Blumenstock, Frank Hase, Thorsten Warneke, Zhiting Wang, Rigel Kivi, and John Robinson
Atmos. Meas. Tech., 9, 4843–4859, https://doi.org/10.5194/amt-9-4843-2016, https://doi.org/10.5194/amt-9-4843-2016, 2016
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Our evaluation of column-averaged methane (XCH4) in models and TCCON reveals latitudinal biases between 0.4 % and 2.1 % originating from an inter-model spread in stratospheric CH4. Substituting model stratospheric CH4 fields by satellite data significantly reduces the large XCH4 bias observed for one model. For other models, showing only minor biases, the impact is ambiguous; i.e., the satellite uncertainty range hinders a more accurate model evaluation needed to improve inverse modeling.
Christoph Zellweger, Lukas Emmenegger, Mohd Firdaus, Juha Hatakka, Martin Heimann, Elena Kozlova, T. Gerard Spain, Martin Steinbacher, Marcel V. van der Schoot, and Brigitte Buchmann
Atmos. Meas. Tech., 9, 4737–4757, https://doi.org/10.5194/amt-9-4737-2016, https://doi.org/10.5194/amt-9-4737-2016, 2016
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We compared instruments using more traditional techniques for measuring CO2 and CH4 at different stations of the Global Atmosphere Watch (GAW) programme with a travelling instrument using a spectroscopic technique. Our results show that the newer analytical techniques have clear advantages over the traditional methods which will lead to the improved accuracy of atmospheric CO2 and CH4 measurement. The work was carried out in the framework of the GAW quality assurance/quality control system.
Matthias Egger, Peter Kraal, Tom Jilbert, Fatimah Sulu-Gambari, Célia J. Sapart, Thomas Röckmann, and Caroline P. Slomp
Biogeosciences, 13, 5333–5355, https://doi.org/10.5194/bg-13-5333-2016, https://doi.org/10.5194/bg-13-5333-2016, 2016
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By combining detailed geochemical analyses with diagenetic modeling, we provide new insights into how methane dynamics may strongly overprint burial records of iron, sulfur and phosphorus in marine systems subject to changes in organic matter loading or water column salinity. A better understanding of these processes will improve our ability to read ancient sediment records and thus to predict the potential consequences of global warming and human-enhanced inputs of nutrients to the ocean.
E. N. Koffi, P. Bergamaschi, U. Karstens, M. Krol, A. Segers, M. Schmidt, I. Levin, A. T. Vermeulen, R. E. Fisher, V. Kazan, H. Klein Baltink, D. Lowry, G. Manca, H. A. J. Meijer, J. Moncrieff, S. Pal, M. Ramonet, H. A. Scheeren, and A. G. Williams
Geosci. Model Dev., 9, 3137–3160, https://doi.org/10.5194/gmd-9-3137-2016, https://doi.org/10.5194/gmd-9-3137-2016, 2016
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We evaluate the capability of the TM5 model to reproduce observations of the boundary layer dynamics and the associated variability of trace gases close to the surface, using 222Rn. Focusing on the European scale, we compare the TM5 boundary layer heights with observations from radiosondes, lidar, and ceilometer. Furthermore, we compare TM5 simulations of 222Rn activity concentrations, using a novel, process-based 222Rn flux map over Europe, with 222Rn harmonized measurements from 10 stations.
Aki Tsuruta, Tuula Aalto, Leif Backman, Janne Hakkarainen, Ingrid T. van der Laan-Luijkx, Maarten C. Krol, Renato Spahni, Sander Houweling, Marko Laine, Marcel van der Schoot, Ray Langenfelds, Raymond Ellul, and Wouter Peters
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2016-181, https://doi.org/10.5194/gmd-2016-181, 2016
Revised manuscript has not been submitted
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In this study, we found that methane emission estimates, driven by the CTE-CH4 model, depend on model setups and inputs, especially for regional estimates. An optimal setup makes the estimates stable, but inputs, such as emission estimates from inventories, and observations, also play significant role. The results can be used for an extended analysis on relative contributions of methane emissions to atmospheric methane concentration changes in recent decades.
Peter Sperlich, Nelly A. M. Uitslag, Jürgen M. Richter, Michael Rothe, Heike Geilmann, Carina van der Veen, Thomas Röckmann, Thomas Blunier, and Willi A. Brand
Atmos. Meas. Tech., 9, 3717–3737, https://doi.org/10.5194/amt-9-3717-2016, https://doi.org/10.5194/amt-9-3717-2016, 2016
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Isotope measurements in atmospheric CH4 are performed since more than 3 decades. However, standard gases to harmonize global measurements are not available to this day. We designed two methods to calibrate a suite of 8 CH4 gases with a wide range in isotopic composition to the VPDB and VSMOW scales with high precision and accuracy. Synthetic air mixtures with ~2 ppm of calibrated CH4 can be provided to the community by the ISOLAB of the Max Planck Institute for Biogeochemistry in Jena, Germany.
Tesfaye Ayalneh Berhanu, Ece Satar, Rudiger Schanda, Peter Nyfeler, Hanspeter Moret, Dominik Brunner, Brian Oney, and Markus Leuenberger
Atmos. Meas. Tech., 9, 2603–2614, https://doi.org/10.5194/amt-9-2603-2016, https://doi.org/10.5194/amt-9-2603-2016, 2016
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In this manuscript, we have presented Co, CO2 and CH4 measurement data from an old radio tower tower (217.5 m) at Beromunster, Switzerland. From about 2 years of continuous CO, CO2 and CH4 measurement at five different heights, we have determined a long-term reproducibility of 2.79 ppb, 0.05 ppm and 0.29 ppb for CO, CO2 and CH4, respectively, compliant with the GAW requirements. We have also observed seasonal and diurnal variation of these species.
Ece Satar, Tesfaye A. Berhanu, Dominik Brunner, Stephan Henne, and Markus Leuenberger
Biogeosciences, 13, 2623–2635, https://doi.org/10.5194/bg-13-2623-2016, https://doi.org/10.5194/bg-13-2623-2016, 2016
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Beromünster tall tower is the flagship of the densely placed Swiss greenhouse gas observation network (CarboCount CH). In this research article we report the first 2 years of the continuous greenhouse gas measurements using cavity ring down spectroscopy analyzer from this tall tower. We have adopted a purely observation based, multi-species and multi-level approach to characterize the site with respect to sources and sinks of natural and anthropogenic origin at diurnal to annual timescales.
Sudhanshu Pandey, Sander Houweling, Maarten Krol, Ilse Aben, Frédéric Chevallier, Edward J. Dlugokencky, Luciana V. Gatti, Emanuel Gloor, John B. Miller, Rob Detmers, Toshinobu Machida, and Thomas Röckmann
Atmos. Chem. Phys., 16, 5043–5062, https://doi.org/10.5194/acp-16-5043-2016, https://doi.org/10.5194/acp-16-5043-2016, 2016
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This study investigates the constraint provided by measurements of Xratio (XCH4/XCO2) from space on surface fluxes of CH4 and CO2. We apply the ratio inversion method described in Pandey et al. (2015) to Xratio retrievals from the GOSAT with the TM5-4DVAR inverse modeling system, to constrain the surface fluxes of CH4 and CO2 for 2009 and 2010. The results are compared to proxy CH4 inversions using model-derived-XCO2 mixing ratios from CarbonTracker and MACC.
Antoine Berchet, Philippe Bousquet, Isabelle Pison, Robin Locatelli, Frédéric Chevallier, Jean-Daniel Paris, Ed J. Dlugokencky, Tuomas Laurila, Juha Hatakka, Yrjo Viisanen, Doug E. J. Worthy, Euan Nisbet, Rebecca Fisher, James France, David Lowry, Viktor Ivakhov, and Ove Hermansen
Atmos. Chem. Phys., 16, 4147–4157, https://doi.org/10.5194/acp-16-4147-2016, https://doi.org/10.5194/acp-16-4147-2016, 2016
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We propose insights based on atmospheric observations around the Arctic circle to evaluate estimates of methane emissions to the atmosphere from the East Siberian Arctic Shelf. Based on a comprehensive statistical analysis of the observations and of high-resolution transport simulations, annual methane emissions from ESAS are estimated to range from 0.0 to 4.5 TgCH4 yr−1, with a maximum in summer and very low emissions in winter.
Stephan Henne, Dominik Brunner, Brian Oney, Markus Leuenberger, Werner Eugster, Ines Bamberger, Frank Meinhardt, Martin Steinbacher, and Lukas Emmenegger
Atmos. Chem. Phys., 16, 3683–3710, https://doi.org/10.5194/acp-16-3683-2016, https://doi.org/10.5194/acp-16-3683-2016, 2016
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Greenhouse gas emissions can be assessed by "top-down" methods that combine atmospheric observations, a transport model and a mathematical optimisation framework. Here, we apply such a top-down method to the methane emissions of Switzerland, utilising observations from the recently installed CarboCount-CH network. Our Swiss total emissions largely agree with those of the national "bottom-up" inventory, whereas regional differences suggest lower than reported emissions from manure handling.
S. Eyer, B. Tuzson, M. E. Popa, C. van der Veen, T. Röckmann, M. Rothe, W. A. Brand, R. Fisher, D. Lowry, E. G. Nisbet, M. S. Brennwald, E. Harris, C. Zellweger, L. Emmenegger, H. Fischer, and J. Mohn
Atmos. Meas. Tech., 9, 263–280, https://doi.org/10.5194/amt-9-263-2016, https://doi.org/10.5194/amt-9-263-2016, 2016
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We present a newly developed field-deployable, autonomous platform simultaneously measuring the three most abundant isotopologues of methane using mid-infrared laser absorption spectroscopy.
The instrument consists of a compact quantum cascade laser absorption spectrometer (QCLAS) coupled to a preconcentration unit, called TRace gas EXtractor (TREX).
The performance of this new in situ technique was investigated during a 2-week measurement campaign and compared to other techniques.
N. Bândă, M. Krol, M. van Weele, T. van Noije, P. Le Sager, and T. Röckmann
Atmos. Chem. Phys., 16, 195–214, https://doi.org/10.5194/acp-16-195-2016, https://doi.org/10.5194/acp-16-195-2016, 2016
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We quantify the processes responsible for methane growth rate variability in the period 1990 to 1995, a period with variations in climate and radiation due to the Pinatubo eruption. We find significant contributions from changes in the methane emission from wetlands, and in the methane removal by OH caused by stratospheric aerosols, by the decrease in temperature and water vapour, by stratospheric ozone depletion and by changes in emissions of CO and NMVOC.
S. Walter, A. Kock, T. Steinhoff, B. Fiedler, P. Fietzek, J. Kaiser, M. Krol, M. E. Popa, Q. Chen, T. Tanhua, and T. Röckmann
Biogeosciences, 13, 323–340, https://doi.org/10.5194/bg-13-323-2016, https://doi.org/10.5194/bg-13-323-2016, 2016
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Oceans are a source of H2, an indirect greenhouse gas. Measurements constraining the temporal and spatial patterns of oceanic H2 emissions are sparse and although H2 is assumed to be produced mainly biologically, direct evidence for biogenic marine production was lacking. By analyzing the H2 isotopic composition (δD) we were able to constrain the global H2 budget in more detail, verify biogenic production and point to additional sources. We also showed that current models are reasonably working.
S. L. Pathirana, C. van der Veen, M. E. Popa, and T. Röckmann
Atmos. Meas. Tech., 8, 5315–5324, https://doi.org/10.5194/amt-8-5315-2015, https://doi.org/10.5194/amt-8-5315-2015, 2015
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CO is established as an important indirect greenhouse gas, as it is the major sink for the OH∙. We have developed a fully automated system for the determination of δ13C and δ18O in atmospheric CO. The blank signal of the Schütze reagent is 1-3 % of the typical sample size. The repeatability is 0.1 ‰ for δ13C and 0.2 ‰ for δ18O. The analytical repeatability for the mole fraction is ~0.7 nmol mol-1 for 100 mL of ambient air (185.4 nmol mol-1 of CO). A single measurement is performed in 18 min.
Q. Chen, M. E. Popa, A. M. Batenburg, and T. Röckmann
Atmos. Chem. Phys., 15, 13003–13021, https://doi.org/10.5194/acp-15-13003-2015, https://doi.org/10.5194/acp-15-13003-2015, 2015
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We investigated soil production and uptake of H2 and associated isotope effects. Uptake and emission of H2 occurred simultaneously at all sampling sites, with strongest emission where N2 fixing legume was present. The fractionation constant during soil uptake was about 0.945 and it did not show positive correlation with deposition velocity. The isotopic composition of H2 emitted from soil with legume was about -530‰, which is less deuterium-depleted than isotope equilibrium between H2O and H2.
B. Oney, S. Henne, N. Gruber, M. Leuenberger, I. Bamberger, W. Eugster, and D. Brunner
Atmos. Chem. Phys., 15, 11147–11164, https://doi.org/10.5194/acp-15-11147-2015, https://doi.org/10.5194/acp-15-11147-2015, 2015
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We present a detailed analysis of a new greenhouse gas measurement network
in the Swiss Plateau, situated between the Jura mountains and the Alps. We
find the network's measurements to be information rich and suitable
for studying surface carbon fluxes of the study region. However, we are
limited by the high-resolution (2km) atmospheric transport model's ability
to simulate meteorology at the individual measurement stations, especially
at those situated in rough terrain.
A. Babenhauserheide, S. Basu, S. Houweling, W. Peters, and A. Butz
Atmos. Chem. Phys., 15, 9747–9763, https://doi.org/10.5194/acp-15-9747-2015, https://doi.org/10.5194/acp-15-9747-2015, 2015
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We compare two different data assimilation systems for estimating sources and sinks of CO_2 from concentration measurements. The systems are CarbonTracker and TM5-4DVar, which have both been used in a number of scientific studies. We analyze the differences between both models as well as the sensitivity of the estimated sources and sinks to the observation coverage. The results provide a lower limit for the uncertainty of surface carbon fluxes with the current measurement network.
G. van der Wel, H. Fischer, H. Oerter, H. Meyer, and H. A. J. Meijer
The Cryosphere, 9, 1601–1616, https://doi.org/10.5194/tc-9-1601-2015, https://doi.org/10.5194/tc-9-1601-2015, 2015
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The diffusion of the stable water isotope signal during firnification of snow is a temperature-dependent process. Therefore, past local temperatures can be derived from the differential diffusion length. In this paper we develop a new method for determining this quantity and compare it with the existing method. Both methods are applied to a large number of synthetic data sets to assess the precision and accuracy of the reconstruction and to a section of the Antarctic EDML ice core record.
J.-L. Tison, M. de Angelis, G. Littot, E. Wolff, H. Fischer, M. Hansson, M. Bigler, R. Udisti, A. Wegner, J. Jouzel, B. Stenni, S. Johnsen, V. Masson-Delmotte, A. Landais, V. Lipenkov, L. Loulergue, J.-M. Barnola, J.-R. Petit, B. Delmonte, G. Dreyfus, D. Dahl-Jensen, G. Durand, B. Bereiter, A. Schilt, R. Spahni, K. Pol, R. Lorrain, R. Souchez, and D. Samyn
The Cryosphere, 9, 1633–1648, https://doi.org/10.5194/tc-9-1633-2015, https://doi.org/10.5194/tc-9-1633-2015, 2015
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The oldest paleoclimatic information is buried within the lowermost layers of deep ice cores. It is therefore essential to judge how deep these records remain unaltered. We study the bottom 60 meters of the EPICA Dome C ice core from central Antarctica to show that the paleoclimatic signal is only affected at the small scale (decimeters) in terms of some of the global ice properties. However our data suggest that the time scale has been considerably distorted by mechanical stretching.
S. Pandey, S. Houweling, M. Krol, I. Aben, and T. Röckmann
Atmos. Chem. Phys., 15, 8615–8629, https://doi.org/10.5194/acp-15-8615-2015, https://doi.org/10.5194/acp-15-8615-2015, 2015
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This study attempts to determine the feasibility of a new assimilation method of satellite measurements of CH4 and CO2 for optimization of their surface fluxes in a synthetic environment. Instead of their absolute concentrations, we assimilate the ratios of their concentrations (CH4/CO2) in our inversion. Doing so helps us to reduce the effect of atmospheric scattering on the measurements in our system. However, assimilation of the ratios makes the inversion non-linear.
K. Ishijima, M. Takigawa, K. Sudo, S. Toyoda, N. Yoshida, T. Röckmann, J. Kaiser, S. Aoki, S. Morimoto, S. Sugawara, and T. Nakazawa
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-15-19947-2015, https://doi.org/10.5194/acpd-15-19947-2015, 2015
Revised manuscript not accepted
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We developed an atmospheric N2O isotopocule model based on a chemistry-coupled atmospheric general circulation model and a simple method to optimize the model, and estimated the isotopic signatures of surface sources at the hemispheric scale. Data obtained from ground-based observations, measurements of firn air, and balloon and aircraft flights were used to optimize the long-term trends, interhemispheric gradients, and photolytic fractionation, respectively, in the model.
S. J. Allin, J. C. Laube, E. Witrant, J. Kaiser, E. McKenna, P. Dennis, R. Mulvaney, E. Capron, P. Martinerie, T. Röckmann, T. Blunier, J. Schwander, P. J. Fraser, R. L. Langenfelds, and W. T. Sturges
Atmos. Chem. Phys., 15, 6867–6877, https://doi.org/10.5194/acp-15-6867-2015, https://doi.org/10.5194/acp-15-6867-2015, 2015
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Stratospheric ozone protects life on Earth from harmful UV-B radiation. Chlorofluorocarbons (CFCs) are man-made compounds which act to destroy this barrier.
This paper presents (1) the first measurements of the stratospheric δ(37Cl) of CFCs -11 and -113; (2) the first quantification of long-term trends in the tropospheric δ(37Cl) of CFCs -11, -12 and -113.
This study provides a better understanding of source and sink processes associated with these destructive compounds.
B. Wolf, L. Merbold, C. Decock, B. Tuzson, E. Harris, J. Six, L. Emmenegger, and J. Mohn
Biogeosciences, 12, 2517–2531, https://doi.org/10.5194/bg-12-2517-2015, https://doi.org/10.5194/bg-12-2517-2015, 2015
F. A. Stap, O. P. Hasekamp, and T. Röckmann
Atmos. Meas. Tech., 8, 1287–1301, https://doi.org/10.5194/amt-8-1287-2015, https://doi.org/10.5194/amt-8-1287-2015, 2015
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We present the capability of an aerosol retrieval algorithm, intended for multi-angle, multi-wavelength photopolarimetric measurements, to intrinsically screen for sub-pixel liquid water cloud contamination.
The screening is based on goodness-of-fit criteria. The algorithm has been applied to a synthetic data set of partially clouded scenes and (non-cloud-screened) POLDER3/PARASOL observations.
S. J. Sutanto, G. Hoffmann, R. A. Scheepmaker, J. Worden, S. Houweling, K. Yoshimura, I. Aben, and T. Röckmann
Atmos. Meas. Tech., 8, 999–1019, https://doi.org/10.5194/amt-8-999-2015, https://doi.org/10.5194/amt-8-999-2015, 2015
D. J. Mrozek, C. van der Veen, M. Kliphuis, J. Kaiser, A. A. Wiegel, and T. Röckmann
Atmos. Meas. Tech., 8, 811–822, https://doi.org/10.5194/amt-8-811-2015, https://doi.org/10.5194/amt-8-811-2015, 2015
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Our analytical system is a promising tool for investigating the triple oxygen isotope composition of CO2 from stratospheric air samples of volumes 100ml and smaller. The method is designed for measuring air samples with CO2 mole fractions between 360 and 400ppm, and it is the first fully automated analytical system that uses CeO2 as the isotope exchange medium.
P. Bergamaschi, M. Corazza, U. Karstens, M. Athanassiadou, R. L. Thompson, I. Pison, A. J. Manning, P. Bousquet, A. Segers, A. T. Vermeulen, G. Janssens-Maenhout, M. Schmidt, M. Ramonet, F. Meinhardt, T. Aalto, L. Haszpra, J. Moncrieff, M. E. Popa, D. Lowry, M. Steinbacher, A. Jordan, S. O'Doherty, S. Piacentino, and E. Dlugokencky
Atmos. Chem. Phys., 15, 715–736, https://doi.org/10.5194/acp-15-715-2015, https://doi.org/10.5194/acp-15-715-2015, 2015
S. J. O'Shea, G. Allen, M. W. Gallagher, K. Bower, S. M. Illingworth, J. B. A. Muller, B. T. Jones, C. J. Percival, S. J-B. Bauguitte, M. Cain, N. Warwick, A. Quiquet, U. Skiba, J. Drewer, K. Dinsmore, E. G. Nisbet, D. Lowry, R. E. Fisher, J. L. France, M. Aurela, A. Lohila, G. Hayman, C. George, D. B. Clark, A. J. Manning, A. D. Friend, and J. Pyle
Atmos. Chem. Phys., 14, 13159–13174, https://doi.org/10.5194/acp-14-13159-2014, https://doi.org/10.5194/acp-14-13159-2014, 2014
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This paper presents airborne measurements of greenhouse gases collected in the European Arctic. Regional scale flux estimates for the northern Scandinavian wetlands are derived. These fluxes are found to be in excellent agreement with coincident surface measurements within the aircraft's sampling domain. This has allowed a significant low bias to be identified in two commonly used process-based land surface models.
M. Riederer, J. Hübner, J. Ruppert, W. A. Brand, and T. Foken
Atmos. Meas. Tech., 7, 4237–4250, https://doi.org/10.5194/amt-7-4237-2014, https://doi.org/10.5194/amt-7-4237-2014, 2014
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The REA technique cannot be applied on grassland shortly after management without the risk of REA-flux errors due to large uncertainties of b-factors and lacking scalar similarity.
The NEE flux partitioning model based on REA measurement results is complex but can enhance results of common partitioning by considering ecosystem discrimination of 13C and wind velocity.
S. Henning, K. Dieckmann, K. Ignatius, M. Schäfer, P. Zedler, E. Harris, B. Sinha, D. van Pinxteren, S. Mertes, W. Birmili, M. Merkel, Z. Wu, A. Wiedensohler, H. Wex, H. Herrmann, and F. Stratmann
Atmos. Chem. Phys., 14, 7859–7868, https://doi.org/10.5194/acp-14-7859-2014, https://doi.org/10.5194/acp-14-7859-2014, 2014
S. J. Sutanto, B. van den Hurk, P. A. Dirmeyer, S. I. Seneviratne, T. Röckmann, K. E. Trenberth, E. M. Blyth, J. Wenninger, and G. Hoffmann
Hydrol. Earth Syst. Sci., 18, 2815–2827, https://doi.org/10.5194/hess-18-2815-2014, https://doi.org/10.5194/hess-18-2815-2014, 2014
M. Bock, J. Schmitt, J. Beck, R. Schneider, and H. Fischer
Atmos. Meas. Tech., 7, 1999–2012, https://doi.org/10.5194/amt-7-1999-2014, https://doi.org/10.5194/amt-7-1999-2014, 2014
U. Dusek, M. Monaco, M. Prokopiou, F. Gongriep, R. Hitzenberger, H. A. J. Meijer, and T. Röckmann
Atmos. Meas. Tech., 7, 1943–1955, https://doi.org/10.5194/amt-7-1943-2014, https://doi.org/10.5194/amt-7-1943-2014, 2014
R. L. Thompson, K. Ishijima, E. Saikawa, M. Corazza, U. Karstens, P. K. Patra, P. Bergamaschi, F. Chevallier, E. Dlugokencky, R. G. Prinn, R. F. Weiss, S. O'Doherty, P. J. Fraser, L. P. Steele, P. B. Krummel, A. Vermeulen, Y. Tohjima, A. Jordan, L. Haszpra, M. Steinbacher, S. Van der Laan, T. Aalto, F. Meinhardt, M. E. Popa, J. Moncrieff, and P. Bousquet
Atmos. Chem. Phys., 14, 6177–6194, https://doi.org/10.5194/acp-14-6177-2014, https://doi.org/10.5194/acp-14-6177-2014, 2014
A. J. van Beelen, G. J. H. Roelofs, O. P. Hasekamp, J. S. Henzing, and T. Röckmann
Atmos. Chem. Phys., 14, 5969–5987, https://doi.org/10.5194/acp-14-5969-2014, https://doi.org/10.5194/acp-14-5969-2014, 2014
O. Peltola, A. Hensen, C. Helfter, L. Belelli Marchesini, F. C. Bosveld, W. C. M. van den Bulk, J. A. Elbers, S. Haapanala, J. Holst, T. Laurila, A. Lindroth, E. Nemitz, T. Röckmann, A. T. Vermeulen, and I. Mammarella
Biogeosciences, 11, 3163–3186, https://doi.org/10.5194/bg-11-3163-2014, https://doi.org/10.5194/bg-11-3163-2014, 2014
M. Baumgartner, P. Kindler, O. Eicher, G. Floch, A. Schilt, J. Schwander, R. Spahni, E. Capron, J. Chappellaz, M. Leuenberger, H. Fischer, and T. F. Stocker
Clim. Past, 10, 903–920, https://doi.org/10.5194/cp-10-903-2014, https://doi.org/10.5194/cp-10-903-2014, 2014
E. Harris, B. Sinha, D. van Pinxteren, J. Schneider, L. Poulain, J. Collett, B. D'Anna, B. Fahlbusch, S. Foley, K. W. Fomba, C. George, T. Gnauk, S. Henning, T. Lee, S. Mertes, A. Roth, F. Stratmann, S. Borrmann, P. Hoppe, and H. Herrmann
Atmos. Chem. Phys., 14, 4219–4235, https://doi.org/10.5194/acp-14-4219-2014, https://doi.org/10.5194/acp-14-4219-2014, 2014
S. Houweling, M. Krol, P. Bergamaschi, C. Frankenberg, E. J. Dlugokencky, I. Morino, J. Notholt, V. Sherlock, D. Wunch, V. Beck, C. Gerbig, H. Chen, E. A. Kort, T. Röckmann, and I. Aben
Atmos. Chem. Phys., 14, 3991–4012, https://doi.org/10.5194/acp-14-3991-2014, https://doi.org/10.5194/acp-14-3991-2014, 2014
R. V. Hiller, D. Bretscher, T. DelSontro, T. Diem, W. Eugster, R. Henneberger, S. Hobi, E. Hodson, D. Imer, M. Kreuzer, T. Künzle, L. Merbold, P. A. Niklaus, B. Rihm, A. Schellenberger, M. H. Schroth, C. J. Schubert, H. Siegrist, J. Stieger, N. Buchmann, and D. Brunner
Biogeosciences, 11, 1941–1959, https://doi.org/10.5194/bg-11-1941-2014, https://doi.org/10.5194/bg-11-1941-2014, 2014
B. Ringeval, S. Houweling, P. M. van Bodegom, R. Spahni, R. van Beek, F. Joos, and T. Röckmann
Biogeosciences, 11, 1519–1558, https://doi.org/10.5194/bg-11-1519-2014, https://doi.org/10.5194/bg-11-1519-2014, 2014
C. Weaver, C. Kiemle, S. R. Kawa, T. Aalto, J. Necki, M. Steinbacher, J. Arduini, F. Apadula, H. Berkhout, and J. Hatakka
Atmos. Chem. Phys., 14, 2625–2637, https://doi.org/10.5194/acp-14-2625-2014, https://doi.org/10.5194/acp-14-2625-2014, 2014
M. E. Popa, M. K. Vollmer, A. Jordan, W. A. Brand, S. L. Pathirana, M. Rothe, and T. Röckmann
Atmos. Chem. Phys., 14, 2105–2123, https://doi.org/10.5194/acp-14-2105-2014, https://doi.org/10.5194/acp-14-2105-2014, 2014
D. Helmig, V. Petrenko, P. Martinerie, E. Witrant, T. Röckmann, A. Zuiderweg, R. Holzinger, J. Hueber, C. Thompson, J. W. C. White, W. Sturges, A. Baker, T. Blunier, D. Etheridge, M. Rubino, and P. Tans
Atmos. Chem. Phys., 14, 1463–1483, https://doi.org/10.5194/acp-14-1463-2014, https://doi.org/10.5194/acp-14-1463-2014, 2014
A. Baklanov, K. Schlünzen, P. Suppan, J. Baldasano, D. Brunner, S. Aksoyoglu, G. Carmichael, J. Douros, J. Flemming, R. Forkel, S. Galmarini, M. Gauss, G. Grell, M. Hirtl, S. Joffre, O. Jorba, E. Kaas, M. Kaasik, G. Kallos, X. Kong, U. Korsholm, A. Kurganskiy, J. Kushta, U. Lohmann, A. Mahura, A. Manders-Groot, A. Maurizi, N. Moussiopoulos, S. T. Rao, N. Savage, C. Seigneur, R. S. Sokhi, E. Solazzo, S. Solomos, B. Sørensen, G. Tsegas, E. Vignati, B. Vogel, and Y. Zhang
Atmos. Chem. Phys., 14, 317–398, https://doi.org/10.5194/acp-14-317-2014, https://doi.org/10.5194/acp-14-317-2014, 2014
S. Schüpbach, U. Federer, P. R. Kaufmann, S. Albani, C. Barbante, T. F. Stocker, and H. Fischer
Clim. Past, 9, 2789–2807, https://doi.org/10.5194/cp-9-2789-2013, https://doi.org/10.5194/cp-9-2789-2013, 2013
R. Schneider, J. Schmitt, P. Köhler, F. Joos, and H. Fischer
Clim. Past, 9, 2507–2523, https://doi.org/10.5194/cp-9-2507-2013, https://doi.org/10.5194/cp-9-2507-2013, 2013
H. Fischer, J. Severinghaus, E. Brook, E. Wolff, M. Albert, O. Alemany, R. Arthern, C. Bentley, D. Blankenship, J. Chappellaz, T. Creyts, D. Dahl-Jensen, M. Dinn, M. Frezzotti, S. Fujita, H. Gallee, R. Hindmarsh, D. Hudspeth, G. Jugie, K. Kawamura, V. Lipenkov, H. Miller, R. Mulvaney, F. Parrenin, F. Pattyn, C. Ritz, J. Schwander, D. Steinhage, T. van Ommen, and F. Wilhelms
Clim. Past, 9, 2489–2505, https://doi.org/10.5194/cp-9-2489-2013, https://doi.org/10.5194/cp-9-2489-2013, 2013
R. Locatelli, P. Bousquet, F. Chevallier, A. Fortems-Cheney, S. Szopa, M. Saunois, A. Agusti-Panareda, D. Bergmann, H. Bian, P. Cameron-Smith, M. P. Chipperfield, E. Gloor, S. Houweling, S. R. Kawa, M. Krol, P. K. Patra, R. G. Prinn, M. Rigby, R. Saito, and C. Wilson
Atmos. Chem. Phys., 13, 9917–9937, https://doi.org/10.5194/acp-13-9917-2013, https://doi.org/10.5194/acp-13-9917-2013, 2013
F. A. Haumann, A. M. Batenburg, G. Pieterse, C. Gerbig, M. C. Krol, and T. Röckmann
Atmos. Chem. Phys., 13, 9401–9413, https://doi.org/10.5194/acp-13-9401-2013, https://doi.org/10.5194/acp-13-9401-2013, 2013
M. von Hobe, S. Bekki, S. Borrmann, F. Cairo, F. D'Amato, G. Di Donfrancesco, A. Dörnbrack, A. Ebersoldt, M. Ebert, C. Emde, I. Engel, M. Ern, W. Frey, S. Genco, S. Griessbach, J.-U. Grooß, T. Gulde, G. Günther, E. Hösen, L. Hoffmann, V. Homonnai, C. R. Hoyle, I. S. A. Isaksen, D. R. Jackson, I. M. Jánosi, R. L. Jones, K. Kandler, C. Kalicinsky, A. Keil, S. M. Khaykin, F. Khosrawi, R. Kivi, J. Kuttippurath, J. C. Laube, F. Lefèvre, R. Lehmann, S. Ludmann, B. P. Luo, M. Marchand, J. Meyer, V. Mitev, S. Molleker, R. Müller, H. Oelhaf, F. Olschewski, Y. Orsolini, T. Peter, K. Pfeilsticker, C. Piesch, M. C. Pitts, L. R. Poole, F. D. Pope, F. Ravegnani, M. Rex, M. Riese, T. Röckmann, B. Rognerud, A. Roiger, C. Rolf, M. L. Santee, M. Scheibe, C. Schiller, H. Schlager, M. Siciliani de Cumis, N. Sitnikov, O. A. Søvde, R. Spang, N. Spelten, F. Stordal, O. Sumińska-Ebersoldt, A. Ulanovski, J. Ungermann, S. Viciani, C. M. Volk, M. vom Scheidt, P. von der Gathen, K. Walker, T. Wegner, R. Weigel, S. Weinbruch, G. Wetzel, F. G. Wienhold, I. Wohltmann, W. Woiwode, I. A. K. Young, V. Yushkov, B. Zobrist, and F. Stroh
Atmos. Chem. Phys., 13, 9233–9268, https://doi.org/10.5194/acp-13-9233-2013, https://doi.org/10.5194/acp-13-9233-2013, 2013
G. Broquet, F. Chevallier, F.-M. Bréon, N. Kadygrov, M. Alemanno, F. Apadula, S. Hammer, L. Haszpra, F. Meinhardt, J. A. Morguí, J. Necki, S. Piacentino, M. Ramonet, M. Schmidt, R. L. Thompson, A. T. Vermeulen, C. Yver, and P. Ciais
Atmos. Chem. Phys., 13, 9039–9056, https://doi.org/10.5194/acp-13-9039-2013, https://doi.org/10.5194/acp-13-9039-2013, 2013
S. Basu, S. Guerlet, A. Butz, S. Houweling, O. Hasekamp, I. Aben, P. Krummel, P. Steele, R. Langenfelds, M. Torn, S. Biraud, B. Stephens, A. Andrews, and D. Worthy
Atmos. Chem. Phys., 13, 8695–8717, https://doi.org/10.5194/acp-13-8695-2013, https://doi.org/10.5194/acp-13-8695-2013, 2013
P. Sperlich, C. Buizert, T. M. Jenk, C. J. Sapart, M. Prokopiou, T. Röckmann, and T. Blunier
Atmos. Meas. Tech., 6, 2027–2041, https://doi.org/10.5194/amt-6-2027-2013, https://doi.org/10.5194/amt-6-2027-2013, 2013
I. T. van der Laan-Luijkx, S. van der Laan, C. Uglietti, M. F. Schibig, R. E. M. Neubert, H. A. J. Meijer, W. A. Brand, A. Jordan, J. M. Richter, M. Rothe, and M. C. Leuenberger
Atmos. Meas. Tech., 6, 1805–1815, https://doi.org/10.5194/amt-6-1805-2013, https://doi.org/10.5194/amt-6-1805-2013, 2013
A. Berchet, I. Pison, F. Chevallier, P. Bousquet, S. Conil, M. Geever, T. Laurila, J. Lavrič, M. Lopez, J. Moncrieff, J. Necki, M. Ramonet, M. Schmidt, M. Steinbacher, and J. Tarniewicz
Atmos. Chem. Phys., 13, 7115–7132, https://doi.org/10.5194/acp-13-7115-2013, https://doi.org/10.5194/acp-13-7115-2013, 2013
P. Sturm, B. Tuzson, S. Henne, and L. Emmenegger
Atmos. Meas. Tech., 6, 1659–1671, https://doi.org/10.5194/amt-6-1659-2013, https://doi.org/10.5194/amt-6-1659-2013, 2013
J. Schmitt, B. Seth, M. Bock, C. van der Veen, L. Möller, C. J. Sapart, M. Prokopiou, T. Sowers, T. Röckmann, and H. Fischer
Atmos. Meas. Tech., 6, 1425–1445, https://doi.org/10.5194/amt-6-1425-2013, https://doi.org/10.5194/amt-6-1425-2013, 2013
S. Walter, A. Kock, and T. Röckmann
Biogeosciences, 10, 3391–3403, https://doi.org/10.5194/bg-10-3391-2013, https://doi.org/10.5194/bg-10-3391-2013, 2013
S. J. O'Shea, S. J.-B. Bauguitte, M. W. Gallagher, D. Lowry, and C. J. Percival
Atmos. Meas. Tech., 6, 1095–1109, https://doi.org/10.5194/amt-6-1095-2013, https://doi.org/10.5194/amt-6-1095-2013, 2013
B. Tuzson, K. Zeyer, M. Steinbacher, J. B. McManus, D. D. Nelson, M. S. Zahniser, and L. Emmenegger
Atmos. Meas. Tech., 6, 927–936, https://doi.org/10.5194/amt-6-927-2013, https://doi.org/10.5194/amt-6-927-2013, 2013
M. Wendeberg, J. M. Richter, M. Rothe, and W. A. Brand
Atmos. Meas. Tech., 6, 817–822, https://doi.org/10.5194/amt-6-817-2013, https://doi.org/10.5194/amt-6-817-2013, 2013
S. Zürcher, R. Spahni, F. Joos, M. Steinacher, and H. Fischer
Biogeosciences, 10, 1963–1981, https://doi.org/10.5194/bg-10-1963-2013, https://doi.org/10.5194/bg-10-1963-2013, 2013
J. C. Laube, A. Keil, H. Bönisch, A. Engel, T. Röckmann, C. M. Volk, and W. T. Sturges
Atmos. Chem. Phys., 13, 2779–2791, https://doi.org/10.5194/acp-13-2779-2013, https://doi.org/10.5194/acp-13-2779-2013, 2013
N. Bândă, M. Krol, M. van Weele, T. van Noije, and T. Röckmann
Atmos. Chem. Phys., 13, 2267–2281, https://doi.org/10.5194/acp-13-2267-2013, https://doi.org/10.5194/acp-13-2267-2013, 2013
B. Bereiter, T. F. Stocker, and H. Fischer
Atmos. Meas. Tech., 6, 251–262, https://doi.org/10.5194/amt-6-251-2013, https://doi.org/10.5194/amt-6-251-2013, 2013
D. A. Belikov, S. Maksyutov, M. Krol, A. Fraser, M. Rigby, H. Bian, A. Agusti-Panareda, D. Bergmann, P. Bousquet, P. Cameron-Smith, M. P. Chipperfield, A. Fortems-Cheiney, E. Gloor, K. Haynes, P. Hess, S. Houweling, S. R. Kawa, R. M. Law, Z. Loh, L. Meng, P. I. Palmer, P. K. Patra, R. G. Prinn, R. Saito, and C. Wilson
Atmos. Chem. Phys., 13, 1093–1114, https://doi.org/10.5194/acp-13-1093-2013, https://doi.org/10.5194/acp-13-1093-2013, 2013
C. Knote and D. Brunner
Atmos. Chem. Phys., 13, 1177–1192, https://doi.org/10.5194/acp-13-1177-2013, https://doi.org/10.5194/acp-13-1177-2013, 2013
M. van den Broeke, P. Smeets, J. Ettema, C. van der Veen, R. van de Wal, and J. Oerlemans
The Cryosphere, 2, 179–189, https://doi.org/10.5194/tc-2-179-2008, https://doi.org/10.5194/tc-2-179-2008, 2008
Related subject area
Subject: Isotopes | Research Activity: Field Measurements | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
A seasonal analysis of aerosol NO3− sources and NOx oxidation pathways in the Southern Ocean marine boundary layer
Nitrate chemistry in the northeast US – Part 1: Nitrogen isotope seasonality tracks nitrate formation chemistry
Nitrate chemistry in the northeast US – Part 2: Oxygen isotopes reveal differences in particulate and gas-phase formation
Photolytic modification of seasonal nitrate isotope cycles in East Antarctica
Atmospheric methane isotopes identify inventory knowledge gaps in the Surat Basin, Australia, coal seam gas and agricultural regions
Methane (CH4) sources in Krakow, Poland: insights from isotope analysis
Isotopic signatures of major methane sources in the coal seam gas fields and adjacent agricultural districts, Queensland, Australia
Measurement report: Nitrogen isotopes (δ15N) and first quantification of oxygen isotope anomalies (Δ17O, δ18O) in atmospheric nitrogen dioxide
Measurement report: Spatial variability of northern Iberian rainfall stable isotope values – investigating atmospheric controls on daily and monthly timescales
Isotopic constraints on atmospheric sulfate formation pathways in the Mt. Everest region, southern Tibetan Plateau
Baffin Bay sea ice extent and synoptic moisture transport drive water vapor isotope (δ18O, δ2H, and deuterium excess) variability in coastal northwest Greenland
New evidence for atmospheric mercury transformations in the marine boundary layer from stable mercury isotopes
The isotopic composition of atmospheric nitrous oxide observed at the high-altitude research station Jungfraujoch, Switzerland
Deposition, recycling, and archival of nitrate stable isotopes between the air–snow interface: comparison between Dronning Maud Land and Dome C, Antarctica
Oxygen and sulfur mass-independent isotopic signatures in black crusts: the complementary negative Δ33S reservoir of sulfate aerosols?
Atmospheric radiocarbon measurements to quantify CO2 emissions in the UK from 2014 to 2015
An improved estimate for the δ13C and δ18O signatures of carbon monoxide produced from atmospheric oxidation of volatile organic compounds
Seasonality in the Δ33S measured in urban aerosols highlights an additional oxidation pathway for atmospheric SO2
The Δ17O and δ18O values of atmospheric nitrates simultaneously collected downwind of anthropogenic sources – implications for polluted air masses
A very limited role of tropospheric chlorine as a sink of the greenhouse gas methane
Detection and variability of combustion-derived vapor in an urban basin
Stable sulfur isotope measurements to trace the fate of SO2 in the Athabasca oil sands region
Triple oxygen isotopes indicate urbanization affects sources of nitrate in wet and dry atmospheric deposition
Isotopic constraints on heterogeneous sulfate production in Beijing haze
Estimation of the fossil fuel component in atmospheric CO2 based on radiocarbon measurements at the Beromünster tall tower, Switzerland
Constraining N2O emissions since 1940 using firn air isotope measurements in both hemispheres
Seasonal variations of triple oxygen isotopic compositions of atmospheric sulfate, nitrate, and ozone at Dumont d'Urville, coastal Antarctica
Carbon isotopic signature of coal-derived methane emissions to the atmosphere: from coalification to alteration
Isotopic composition for source identification of mercury in atmospheric fine particles
Isotopic constraints on the role of hypohalous acids in sulfate aerosol formation in the remote marine boundary layer
Oxygen isotope mass balance of atmospheric nitrate at Dome C, East Antarctica, during the OPALE campaign
Isotopic effects of nitrate photochemistry in snow: a field study at Dome C, Antarctica
Stable carbon isotope ratios of ambient secondary organic aerosols in Toronto
WAIS Divide ice core suggests sustained changes in the atmospheric formation pathways of sulfate and nitrate since the 19th century in the extratropical Southern Hemisphere
Stable carbon isotope ratios of toluene in the boundary layer and the lower free troposphere
Emission ratio and isotopic signatures of molecular hydrogen emissions from tropical biomass burning
Can the carbon isotopic composition of methane be reconstructed from multi-site firn air measurements?
Air–snow transfer of nitrate on the East Antarctic Plateau – Part 1: Isotopic evidence for a photolytically driven dynamic equilibrium in summer
Chemical characterization and stable carbon isotopic composition of particulate Polycyclic Aromatic Hydrocarbons issued from combustion of 10 Mediterranean woods
Quantification of the carbonaceous matter origin in submicron marine aerosol by 13C and 14C isotope analysis
Temporal and spatial variability of the stable isotopic composition of atmospheric molecular hydrogen: observations at six EUROHYDROS stations
Continuous isotopic composition measurements of tropospheric CO2 at Jungfraujoch (3580 m a.s.l.), Switzerland: real-time observation of regional pollution events
Anthropogenic imprints on nitrogen and oxygen isotopic composition of precipitation nitrate in a nitrogen-polluted city in southern China
Analysis of 13C and 18O isotope data of CO2 in CARIBIC aircraft samples as tracers of upper troposphere/lower stratosphere mixing and the global carbon cycle
Tracing the fate of atmospheric nitrate deposited onto a forest ecosystem in Eastern Asia using Δ17O
Photolysis imprint in the nitrate stable isotope signal in snow and atmosphere of East Antarctica and implications for reactive nitrogen cycling
Sources and transport of Δ14C in CO2 within the Mexico City Basin and vicinity
Jessica M. Burger, Emily Joyce, Meredith G. Hastings, Kurt A. M. Spence, and Katye E. Altieri
Atmos. Chem. Phys., 23, 5605–5622, https://doi.org/10.5194/acp-23-5605-2023, https://doi.org/10.5194/acp-23-5605-2023, 2023
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A seasonal analysis of the nitrogen isotopes of atmospheric nitrate over the remote Southern Ocean reveals that similar natural NOx sources dominate in spring and summer, while winter is representative of background-level conditions. The oxygen isotopes suggest that similar oxidation pathways involving more ozone occur in spring and winter, while the hydroxyl radical is the main oxidant in summer. This work helps to constrain NOx cycling and oxidant budgets in a data-sparse remote marine region.
Claire Bekker, Wendell W. Walters, Lee T. Murray, and Meredith G. Hastings
Atmos. Chem. Phys., 23, 4185–4201, https://doi.org/10.5194/acp-23-4185-2023, https://doi.org/10.5194/acp-23-4185-2023, 2023
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Nitrate is a critical component of the atmosphere that degrades air quality and ecosystem health. We have investigated the nitrogen isotope compositions of nitrate from deposition samples collected across the northeastern United States. Spatiotemporal variability in the nitrogen isotope compositions was found to track with nitrate formation chemistry. Our results highlight that nitrogen isotope compositions may be a robust tool for improving model representation of nitrate chemistry.
Heejeong Kim, Wendell W. Walters, Claire Bekker, Lee T. Murray, and Meredith G. Hastings
Atmos. Chem. Phys., 23, 4203–4219, https://doi.org/10.5194/acp-23-4203-2023, https://doi.org/10.5194/acp-23-4203-2023, 2023
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Atmospheric nitrate has an important impact on human and ecosystem health. We evaluated atmospheric nitrate formation pathways in the northeastern US utilizing oxygen isotope compositions, which indicated a significant difference between the phases of nitrate (i.e., gas vs. particle). Comparing the observations with model simulations indicated that N2O5 hydrolysis chemistry was overpredicted. Our study has important implications for improving atmospheric chemistry model representation.
Pete D. Akers, Joël Savarino, Nicolas Caillon, Olivier Magand, and Emmanuel Le Meur
Atmos. Chem. Phys., 22, 15637–15657, https://doi.org/10.5194/acp-22-15637-2022, https://doi.org/10.5194/acp-22-15637-2022, 2022
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Nitrate isotopes in Antarctic ice do not preserve the seasonal isotopic cycles of the atmosphere, which limits their use to study the past. We studied nitrate along an 850 km Antarctic transect to learn how these cycles are changed by sunlight-driven chemistry in the snow. Our findings suggest that the snow accumulation rate and other environmental signals can be extracted from nitrate with the right sampling and analytical approaches.
Bryce F. J. Kelly, Xinyi Lu, Stephen J. Harris, Bruno G. Neininger, Jorg M. Hacker, Stefan Schwietzke, Rebecca E. Fisher, James L. France, Euan G. Nisbet, David Lowry, Carina van der Veen, Malika Menoud, and Thomas Röckmann
Atmos. Chem. Phys., 22, 15527–15558, https://doi.org/10.5194/acp-22-15527-2022, https://doi.org/10.5194/acp-22-15527-2022, 2022
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This study explores using the composition of methane of in-flight atmospheric air samples for greenhouse gas inventory verification. The air samples were collected above one of the largest coal seam gas production regions in the world. Adjacent to these gas fields are coal mines, Australia's largest cattle feedlot, and over 1 million grazing cattle. The results are also used to identify methane mitigation opportunities.
Malika Menoud, Carina van der Veen, Jaroslaw Necki, Jakub Bartyzel, Barbara Szénási, Mila Stanisavljević, Isabelle Pison, Philippe Bousquet, and Thomas Röckmann
Atmos. Chem. Phys., 21, 13167–13185, https://doi.org/10.5194/acp-21-13167-2021, https://doi.org/10.5194/acp-21-13167-2021, 2021
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Using measurements of methane isotopes in ambient air and a 3D atmospheric transport model, in Krakow, Poland, we mainly detected fossil-fuel-related sources, coming from coal mining in Silesia and from the use of natural gas in the city. Emission inventories report large emissions from coal mine activity in Silesia, which is in agreement with our measurements. However, methane sources in the urban area of Krakow related to the use of fossil fuels might be underestimated in the inventories.
Xinyi Lu, Stephen J. Harris, Rebecca E. Fisher, James L. France, Euan G. Nisbet, David Lowry, Thomas Röckmann, Carina van der Veen, Malika Menoud, Stefan Schwietzke, and Bryce F. J. Kelly
Atmos. Chem. Phys., 21, 10527–10555, https://doi.org/10.5194/acp-21-10527-2021, https://doi.org/10.5194/acp-21-10527-2021, 2021
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Many coal seam gas (CSG) facilities in the Surat Basin, Australia, are adjacent to other sources of methane, including agricultural, urban, and natural seeps. This makes it challenging to estimate the amount of methane being emitted into the atmosphere from CSG facilities. This research demonstrates that measurements of the carbon and hydrogen stable isotopic composition of methane can distinguish between and apportion methane emissions from CSG facilities, cattle, and many other sources.
Sarah Albertin, Joël Savarino, Slimane Bekki, Albane Barbero, and Nicolas Caillon
Atmos. Chem. Phys., 21, 10477–10497, https://doi.org/10.5194/acp-21-10477-2021, https://doi.org/10.5194/acp-21-10477-2021, 2021
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We report an efficient method to collect atmospheric NO2 adapted for multi-isotopic analysis and present the first NO2 triple oxygen and double nitrogen isotope measurements. Atmospheric samplings carried out in Grenoble, France, highlight the NO2 isotopic signature sensitivity to the local NOx emissions and chemical regimes. These preliminary results are very promising for using the combination of Δ17O and δ15N of NO2 as a probe of the atmospheric NOx emissions and chemistry.
Ana Moreno, Miguel Iglesias, Cesar Azorin-Molina, Carlos Pérez-Mejías, Miguel Bartolomé, Carlos Sancho, Heather Stoll, Isabel Cacho, Jaime Frigola, Cinta Osácar, Arsenio Muñoz, Antonio Delgado-Huertas, Ileana Bladé, and Françoise Vimeux
Atmos. Chem. Phys., 21, 10159–10177, https://doi.org/10.5194/acp-21-10159-2021, https://doi.org/10.5194/acp-21-10159-2021, 2021
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We present a large and unique dataset of the rainfall isotopic composition at seven sites from northern Iberia to characterize their variability at daily and monthly timescales and to assess the role of climate and geographic factors in the modulation of δ18O values. We found that the origin, moisture uptake along the trajectory and type of precipitation play a key role. These results will help to improve the interpretation of δ18O paleorecords from lacustrine carbonates or speleothems.
Kun Wang, Shohei Hattori, Mang Lin, Sakiko Ishino, Becky Alexander, Kazuki Kamezaki, Naohiro Yoshida, and Shichang Kang
Atmos. Chem. Phys., 21, 8357–8376, https://doi.org/10.5194/acp-21-8357-2021, https://doi.org/10.5194/acp-21-8357-2021, 2021
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Sulfate aerosols play an important climatic role and exert adverse effects on the ecological environment and human health. In this study, we present the triple oxygen isotopic composition of sulfate from the Mt. Everest region, southern Tibetan Plateau, and decipher the formation mechanisms of atmospheric sulfate in this pristine environment. The results indicate the important role of the S(IV) + O3 pathway in atmospheric sulfate formation promoted by conditions of high cloud water pH.
Pete D. Akers, Ben G. Kopec, Kyle S. Mattingly, Eric S. Klein, Douglas Causey, and Jeffrey M. Welker
Atmos. Chem. Phys., 20, 13929–13955, https://doi.org/10.5194/acp-20-13929-2020, https://doi.org/10.5194/acp-20-13929-2020, 2020
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Water vapor isotopes recorded for 2 years in coastal northern Greenland largely reflect changes in sea ice cover, with distinct values when Baffin Bay is ice covered in winter vs. open in summer. Resulting changes in moisture transport, surface winds, and air temperature also modify the isotopes. Local glacial ice may thus preserve past changes in the Baffin Bay sea ice extent, and this will help us better understand how the Arctic environment and water cycle responds to global climate change.
Ben Yu, Lin Yang, Linlin Wang, Hongwei Liu, Cailing Xiao, Yong Liang, Qian Liu, Yongguang Yin, Ligang Hu, Jianbo Shi, and Guibin Jiang
Atmos. Chem. Phys., 20, 9713–9723, https://doi.org/10.5194/acp-20-9713-2020, https://doi.org/10.5194/acp-20-9713-2020, 2020
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We found that Br atoms in the marine boundary layer are the most probable oxidizer that transform gaseous elemental mercury into gaseous oxidized mercury, according to the mercury isotopes in the total gaseous mercury. On the other hand, Br or Cl atoms are not the primary oxidizers that produced oxidized mercury on particles. This study showed that mercury isotopes can provide new evidence that help us to fully understand the transformations of atmospheric mercury.
Longfei Yu, Eliza Harris, Stephan Henne, Sarah Eggleston, Martin Steinbacher, Lukas Emmenegger, Christoph Zellweger, and Joachim Mohn
Atmos. Chem. Phys., 20, 6495–6519, https://doi.org/10.5194/acp-20-6495-2020, https://doi.org/10.5194/acp-20-6495-2020, 2020
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We observed the isotopic composition of nitrous oxide in the unpolluted air at Jungfraujoch for 5 years. Our results indicate a clear seasonal pattern in the isotopic composition, corresponding with that in atmospheric nitrous oxide levels. This is most likely due to temporal variations in both emission processes and air mass sources for Jungfraujoch. Our findings are of importance to global nitrous oxide modelling and to better understanding of long-term trends in atmospheric nitrous oxide.
V. Holly L. Winton, Alison Ming, Nicolas Caillon, Lisa Hauge, Anna E. Jones, Joel Savarino, Xin Yang, and Markus M. Frey
Atmos. Chem. Phys., 20, 5861–5885, https://doi.org/10.5194/acp-20-5861-2020, https://doi.org/10.5194/acp-20-5861-2020, 2020
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The transfer of the nitrogen stable isotopic composition in nitrate between the air and snow at low accumulation sites in Antarctica leaves an UV imprint in the snow. Quantifying how nitrate isotope values change allows us to interpret longer ice core records. Based on nitrate observations and modelling at Kohnen, East Antarctica, the dominant factors controlling the nitrate isotope signature in deep snow layers are the depth of light penetration into the snowpack and the snow accumulation rate.
Isabelle Genot, David Au Yang, Erwan Martin, Pierre Cartigny, Erwann Legendre, and Marc De Rafelis
Atmos. Chem. Phys., 20, 4255–4273, https://doi.org/10.5194/acp-20-4255-2020, https://doi.org/10.5194/acp-20-4255-2020, 2020
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Given their critical impact on radiative forcing, sulfate aerosols have been extensively studied using their isotope signatures (δ34S, ∆33S, ∆36S, δ18O, and ∆17O). A striking observation is that ∆33S > 0 ‰, implying a missing reservoir in the sulfur cycle. Here, we measured ∆33S < 0 ‰ in black crust sulfates (i.e., formed on carbonate walls) that must therefore result from distinct chemical pathway(s) compared to sulfate aerosols, and they may well represent this complementary reservoir.
Angelina Wenger, Katherine Pugsley, Simon O'Doherty, Matt Rigby, Alistair J. Manning, Mark F. Lunt, and Emily D. White
Atmos. Chem. Phys., 19, 14057–14070, https://doi.org/10.5194/acp-19-14057-2019, https://doi.org/10.5194/acp-19-14057-2019, 2019
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We present 14CO2 observations at a background site in Ireland and a tall tower site in the UK. These data have been used to calculate the contribution of fossil fuel sources to atmospheric CO2 mole fractions from the UK and Ireland. 14CO2 emissions from nuclear industry sites in the UK cause a higher uncertainty in the results compared to observations in other locations. The observed ffCO2 at the site was not significantly different from simulated values based on the bottom-up inventory.
Isaac J. Vimont, Jocelyn C. Turnbull, Vasilii V. Petrenko, Philip F. Place, Colm Sweeney, Natasha Miles, Scott Richardson, Bruce H. Vaughn, and James W. C. White
Atmos. Chem. Phys., 19, 8547–8562, https://doi.org/10.5194/acp-19-8547-2019, https://doi.org/10.5194/acp-19-8547-2019, 2019
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Stable isotopes of Carbon Monoxide (CO) and radiocarbon carbon dioxide were measured over three summers at Indianapolis, Indiana, US, and for 1 year at a site thought to be strongly influenced by CO from oxidized volatile organic compounds (VOCs) in South Carolina, US. The Indianapolis results were used to provide an estimate of the carbon and oxygen isotopic signatures of CO produced from oxidized VOCs. This updated estimate agrees well with the data from South Carolina during the summer.
David Au Yang, Pierre Cartigny, Karine Desboeufs, and David Widory
Atmos. Chem. Phys., 19, 3779–3796, https://doi.org/10.5194/acp-19-3779-2019, https://doi.org/10.5194/acp-19-3779-2019, 2019
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Sulfates present in urban aerosols collected worldwide usually exhibit 33S-anomalies whose origin remains unclear. Besides, the sulfate concentration is not very well modelled nowadays, which, coupled with the isotopic composition anomaly on the 33S, would highlight the presence of at least an additional oxidation pathway, different from O2+TMI, O3, OH, H2O2 and NO2. We suggest here the implication of two other possible oxidation pathways.
Martine M. Savard, Amanda S. Cole, Robert Vet, and Anna Smirnoff
Atmos. Chem. Phys., 18, 10373–10389, https://doi.org/10.5194/acp-18-10373-2018, https://doi.org/10.5194/acp-18-10373-2018, 2018
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Improving air quality requires understanding of the atmospheric processes transforming nitrous oxides emitted by human activities into nitrates, an N form that may degrade natural ecosystems. Isotopes (∆17O, δ18O) are characterized in separate wet, particulate and gaseous nitrates for the first time. The gas ranges are distinct from those of the other nitrates, and the plume dynamics emerge as crucial in interpreting the results, which unravel key processes behind the distribution of nitrates.
Sergey Gromov, Carl A. M. Brenninkmeijer, and Patrick Jöckel
Atmos. Chem. Phys., 18, 9831–9843, https://doi.org/10.5194/acp-18-9831-2018, https://doi.org/10.5194/acp-18-9831-2018, 2018
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Using the observational data on 13C (CO) and 13C (CH4) from the extra-tropical Southern Hemisphere (ETSH) and EMAC model we (1) provide an independent, observation-based evaluation of Cl atom concentration variations in the ETSH throughout 1994–2000, (2) show that the role of tropospheric Cl as a sink of CH4 is seriously overestimated in the literature, (3) demonstrate that the 13C/12C ratio of CO is a sensitive indicator for the isotopic composition of reacted CH4 and therefore for its sources.
Richard P. Fiorella, Ryan Bares, John C. Lin, James R. Ehleringer, and Gabriel J. Bowen
Atmos. Chem. Phys., 18, 8529–8547, https://doi.org/10.5194/acp-18-8529-2018, https://doi.org/10.5194/acp-18-8529-2018, 2018
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Fossil fuel combustion produces water; where fossil fuel combustion is concentrated in urban areas, this humidity source may represent ~ 10 % of total humidity. In turn, this water vapor addition may alter urban meteorology, though the contribution of combustion vapor is difficult to measure. Using stable water isotopes, we estimate that up to 16 % of urban humidity may arise from combustion when the atmosphere is stable during winter, and develop recommendations for application in other cities.
Neda Amiri, Roya Ghahreman, Ofelia Rempillo, Travis W. Tokarek, Charles A. Odame-Ankrah, Hans D. Osthoff, and Ann-Lise Norman
Atmos. Chem. Phys., 18, 7757–7780, https://doi.org/10.5194/acp-18-7757-2018, https://doi.org/10.5194/acp-18-7757-2018, 2018
David M. Nelson, Urumu Tsunogai, Dong Ding, Takuya Ohyama, Daisuke D. Komatsu, Fumiko Nakagawa, Izumi Noguchi, and Takashi Yamaguchi
Atmos. Chem. Phys., 18, 6381–6392, https://doi.org/10.5194/acp-18-6381-2018, https://doi.org/10.5194/acp-18-6381-2018, 2018
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Atmospheric nitrate may be produced locally and/or come from upwind regions. To address this issue we measured oxygen and nitrogen isotopes of wet and dry nitrate deposition at nearby urban and rural sites. Our results suggest that, relative to nitrate in wet deposition in urban environments and wet and dry deposition in rural environments, nitrate in dry deposition in urban environments results from local NOx emissions more so than wet deposition, which is transported longer distances.
Pengzhen He, Becky Alexander, Lei Geng, Xiyuan Chi, Shidong Fan, Haicong Zhan, Hui Kang, Guangjie Zheng, Yafang Cheng, Hang Su, Cheng Liu, and Zhouqing Xie
Atmos. Chem. Phys., 18, 5515–5528, https://doi.org/10.5194/acp-18-5515-2018, https://doi.org/10.5194/acp-18-5515-2018, 2018
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We use observations of the oxygen isotopic composition of sulfate aerosol as a fingerprint to quantify various sulfate formation mechanisms during pollution events in Beijing, China. We found that heterogeneous reactions on aerosols dominated sulfate production in general; however, in-cloud reactions would dominate haze sulfate production when cloud liquid water content was high. The findings also suggest the heterogeneity of aerosol acidity should be parameterized in models.
Tesfaye A. Berhanu, Sönke Szidat, Dominik Brunner, Ece Satar, Rüdiger Schanda, Peter Nyfeler, Michael Battaglia, Martin Steinbacher, Samuel Hammer, and Markus Leuenberger
Atmos. Chem. Phys., 17, 10753–10766, https://doi.org/10.5194/acp-17-10753-2017, https://doi.org/10.5194/acp-17-10753-2017, 2017
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Fossil fuel CO2 is the major contributor of anthropogenic CO2 in the atmosphere, and accurate quantification is essential to better understand the carbon cycle. Such accurate quantification can be conducted based on radiocarbon measurements. In this study, we present radiocarbon measurements from a tall tower site in Switzerland. From these measurements, we have observed seasonally varying fossil fuel CO2 contributions and a biospheric CO2 component that varies diurnally and seasonally.
Markella Prokopiou, Patricia Martinerie, Célia J. Sapart, Emmanuel Witrant, Guillaume Monteil, Kentaro Ishijima, Sophie Bernard, Jan Kaiser, Ingeborg Levin, Thomas Blunier, David Etheridge, Ed Dlugokencky, Roderik S. W. van de Wal, and Thomas Röckmann
Atmos. Chem. Phys., 17, 4539–4564, https://doi.org/10.5194/acp-17-4539-2017, https://doi.org/10.5194/acp-17-4539-2017, 2017
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Nitrous oxide is the third most important anthropogenic greenhouse gas with an increasing mole fraction. To understand its natural and anthropogenic sources
we employ isotope measurements. Results show that while the N2O mole fraction increases, its heavy isotope content decreases. The isotopic changes observed underline the dominance of agricultural emissions especially at the early part of the record, whereas in the later decades the contribution from other anthropogenic sources increases.
Sakiko Ishino, Shohei Hattori, Joel Savarino, Bruno Jourdain, Susanne Preunkert, Michel Legrand, Nicolas Caillon, Albane Barbero, Kota Kuribayashi, and Naohiro Yoshida
Atmos. Chem. Phys., 17, 3713–3727, https://doi.org/10.5194/acp-17-3713-2017, https://doi.org/10.5194/acp-17-3713-2017, 2017
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We show the first simultaneous observations of triple oxygen isotopic compositions of atmospheric sulfate, nitrate, and ozone at Dumont d'Urville, coastal Antarctica. The contrasting seasonal trends between oxygen isotopes of ozone and those of sulfate and nitrate indicate that these signatures in sulfate and nitrate are mainly controlled by changes in oxidation chemistry. We also discuss the specific oxidation chemistry induced by the unique phenomena at the site.
Giulia Zazzeri, Dave Lowry, Rebecca E. Fisher, James L. France, Mathias Lanoisellé, Bryce F. J. Kelly, Jaroslaw M. Necki, Charlotte P. Iverach, Elisa Ginty, Miroslaw Zimnoch, Alina Jasek, and Euan G. Nisbet
Atmos. Chem. Phys., 16, 13669–13680, https://doi.org/10.5194/acp-16-13669-2016, https://doi.org/10.5194/acp-16-13669-2016, 2016
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Methane emissions estimates from the coal sector are highly uncertain. Precise δ13C isotopic signatures of methane sources can be used in atmospheric models for a methane budget assessment. Emissions from both underground and opencast coal mines in the UK, Australia and Poland were sampled and isotopically characterised using high-precision measurements of δ13C values. Representative isotopic signatures were provided, taking into account specific ranks of coal and mine type.
Qiang Huang, Jiubin Chen, Weilin Huang, Pingqing Fu, Benjamin Guinot, Xinbin Feng, Lihai Shang, Zhuhong Wang, Zhongwei Wang, Shengliu Yuan, Hongming Cai, Lianfang Wei, and Ben Yu
Atmos. Chem. Phys., 16, 11773–11786, https://doi.org/10.5194/acp-16-11773-2016, https://doi.org/10.5194/acp-16-11773-2016, 2016
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Atmospheric airborne mercury is of particular concern because, once inhaled, both Hg and its vectors might have adverse effects on human beings. In this study, we attempted to identify the sources of PM2.5-Hg in Beijing, China, using Hg isotopic composition. Large range and seasonal variations in both mass-dependent and mass-independent fractionations of Hg isotopes in haze particles demonstrate the usefulness of Hg isotopes for directly tracing the sources and its vectors in the atmosphere.
Qianjie Chen, Lei Geng, Johan A. Schmidt, Zhouqing Xie, Hui Kang, Jordi Dachs, Jihong Cole-Dai, Andrew J. Schauer, Madeline G. Camp, and Becky Alexander
Atmos. Chem. Phys., 16, 11433–11450, https://doi.org/10.5194/acp-16-11433-2016, https://doi.org/10.5194/acp-16-11433-2016, 2016
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The formation mechanisms of sulfate in the marine boundary layer are not well understood, which could result in large uncertainties in aerosol radiative forcing. We measure the oxygen isotopic composition (Δ17O) of sulfate collected in the MBL and analyze with a global transport model. Our results suggest that 33–50 % of MBL sulfate is formed via oxidation of S(IV) by hypohalous acids HOBr / HOCl in the aqueous phase, and the daily-mean HOBr/HOCl concentrations are on the order of 0.01–0.1 ppt.
Joël Savarino, William C. Vicars, Michel Legrand, Suzanne Preunkert, Bruno Jourdain, Markus M. Frey, Alexandre Kukui, Nicolas Caillon, and Jaime Gil Roca
Atmos. Chem. Phys., 16, 2659–2673, https://doi.org/10.5194/acp-16-2659-2016, https://doi.org/10.5194/acp-16-2659-2016, 2016
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Atmospheric nitrate is collected on the East Antarctic ice sheet. Nitrogen and oxygen stable isotopes and concentrations of nitrate are measured. Using a box model, we show that there is s systematic discrepancy between observations and model results. We suggest that this discrepancy probably results from unknown NOx chemistry above the Antarctic ice sheet. However, possible misconception in the stable isotope mass balance is not completely excluded.
T. A. Berhanu, J. Savarino, J. Erbland, W. C. Vicars, S. Preunkert, J. F. Martins, and M. S. Johnson
Atmos. Chem. Phys., 15, 11243–11256, https://doi.org/10.5194/acp-15-11243-2015, https://doi.org/10.5194/acp-15-11243-2015, 2015
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In this field study at Dome C, Antarctica, we investigated the effect of solar UV photolysis on the stable isotopes of nitrate in snow via comparison of two identical snow pits while exposing only one to solar UV. From the difference between the average isotopic fractionations calculated for each pit, we determined a purely photolytic nitrogen isotopic fractionation of -55.8‰, in good agreement with what has been recently determined in a laboratory study.
M. Saccon, A. Kornilova, L. Huang, S. Moukhtar, and J. Rudolph
Atmos. Chem. Phys., 15, 10825–10838, https://doi.org/10.5194/acp-15-10825-2015, https://doi.org/10.5194/acp-15-10825-2015, 2015
E. D. Sofen, B. Alexander, E. J. Steig, M. H. Thiemens, S. A. Kunasek, H. M. Amos, A. J. Schauer, M. G. Hastings, J. Bautista, T. L. Jackson, L. E. Vogel, J. R. McConnell, D. R. Pasteris, and E. S. Saltzman
Atmos. Chem. Phys., 14, 5749–5769, https://doi.org/10.5194/acp-14-5749-2014, https://doi.org/10.5194/acp-14-5749-2014, 2014
J. Wintel, E. Hösen, R. Koppmann, M. Krebsbach, A. Hofzumahaus, and F. Rohrer
Atmos. Chem. Phys., 13, 11059–11071, https://doi.org/10.5194/acp-13-11059-2013, https://doi.org/10.5194/acp-13-11059-2013, 2013
F. A. Haumann, A. M. Batenburg, G. Pieterse, C. Gerbig, M. C. Krol, and T. Röckmann
Atmos. Chem. Phys., 13, 9401–9413, https://doi.org/10.5194/acp-13-9401-2013, https://doi.org/10.5194/acp-13-9401-2013, 2013
C. J. Sapart, P. Martinerie, E. Witrant, J. Chappellaz, R. S. W. van de Wal, P. Sperlich, C. van der Veen, S. Bernard, W. T. Sturges, T. Blunier, J. Schwander, D. Etheridge, and T. Röckmann
Atmos. Chem. Phys., 13, 6993–7005, https://doi.org/10.5194/acp-13-6993-2013, https://doi.org/10.5194/acp-13-6993-2013, 2013
J. Erbland, W. C. Vicars, J. Savarino, S. Morin, M. M. Frey, D. Frosini, E. Vince, and J. M. F. Martins
Atmos. Chem. Phys., 13, 6403–6419, https://doi.org/10.5194/acp-13-6403-2013, https://doi.org/10.5194/acp-13-6403-2013, 2013
A. Guillon, K. Le Ménach, P.-M. Flaud, N. Marchand, H. Budzinski, and E. Villenave
Atmos. Chem. Phys., 13, 2703–2719, https://doi.org/10.5194/acp-13-2703-2013, https://doi.org/10.5194/acp-13-2703-2013, 2013
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Short summary
A dual isotope ratio mass spectrometric system (IRMS) and a quantum cascade laser absorption spectroscopy (QCLAS)-based technique were deployed at the Cabauw experimental site for atmospheric research (CESAR) in the Netherlands and performed in situ, high-frequency (approx. hourly) measurements for a period of more than 5 months, yielding a combined dataset with more than 2500 measurements of both δ13C and δD.
A dual isotope ratio mass spectrometric system (IRMS) and a quantum cascade laser absorption...
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