Articles | Volume 21, issue 16
https://doi.org/10.5194/acp-21-12739-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-21-12739-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
27 Aug 2021
Research article |
| 27 Aug 2021
| 27 Aug 2021
Evidence of a recent decline in UK emissions of hydrofluorocarbons determined by the InTEM inverse model and atmospheric measurements
Alistair J. Manning
CORRESPONDING AUTHOR
Met Office Hadley Centre, Exeter EX1 3PB, UK
Alison L. Redington
Met Office Hadley Centre, Exeter EX1 3PB, UK
Daniel Say
School of Chemistry, University of Bristol, Bristol, UK
Simon O'Doherty
School of Chemistry, University of Bristol, Bristol, UK
Dickon Young
School of Chemistry, University of Bristol, Bristol, UK
Peter G. Simmonds
School of Chemistry, University of Bristol, Bristol, UK
Martin K. Vollmer
Empa, Swiss Federal Laboratories for Materials Science and Technology, Dübendorf, Switzerland
Jens Mühle
Scripps Institution of Oceanography, University of California, San Diego, La Jolla, USA
Jgor Arduini
Department of Pure and Applied Sciences, University of Urbino, Urbino, Italy
Gerard Spain
School of Physics, National University of Ireland Galway, Galway, Ireland
Adam Wisher
School of Chemistry, University of Bristol, Bristol, UK
Michela Maione
Department of Pure and Applied Sciences, University of Urbino, Urbino, Italy
Tanja J. Schuck
Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, Frankfurt, Germany
Kieran Stanley
Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, Frankfurt, Germany
Stefan Reimann
Empa, Swiss Federal Laboratories for Materials Science and Technology, Dübendorf, Switzerland
Andreas Engel
Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, Frankfurt, Germany
Paul B. Krummel
Climate Science Centre, CSIRO Oceans and Atmosphere, Aspendale, Australia
Paul J. Fraser
Climate Science Centre, CSIRO Oceans and Atmosphere, Aspendale, Australia
Christina M. Harth
Scripps Institution of Oceanography, University of California, San Diego, La Jolla, USA
Peter K. Salameh
Scripps Institution of Oceanography, University of California, San Diego, La Jolla, USA
Ray F. Weiss
Scripps Institution of Oceanography, University of California, San Diego, La Jolla, USA
Ray Gluckman
Gluckman Consulting, Cobham, UK
Peter N. Brown
Ricardo Energy & Environment, Gemini Building, Fermi Ave, Harwell, UK
John D. Watterson
Ricardo Energy & Environment, Gemini Building, Fermi Ave, Harwell, UK
Tim Arnold
National Physical Laboratory, Teddington, UK
School of GeoSciences, The University of Edinburgh, Edinburgh, UK
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Emily Dowd, Chris Wilson, Martyn P. Chipperfield, Emanuel Gloor, Alistair Manning, and Ruth Doherty
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Alice E. Ramsden, Anita L. Ganesan, Luke M. Western, Matthew Rigby, Alistair J. Manning, Amy Foulds, James L. France, Patrick Barker, Peter Levy, Daniel Say, Adam Wisher, Tim Arnold, Chris Rennick, Kieran M. Stanley, Dickon Young, and Simon O'Doherty
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Eric Saboya, Giulia Zazzeri, Heather Graven, Alistair J. Manning, and Sylvia Englund Michel
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Mark F. Lunt, Alistair J. Manning, Grant Allen, Tim Arnold, Stéphane J.-B. Bauguitte, Hartmut Boesch, Anita L. Ganesan, Aoife Grant, Carole Helfter, Eiko Nemitz, Simon J. O'Doherty, Paul I. Palmer, Joseph R. Pitt, Chris Rennick, Daniel Say, Kieran M. Stanley, Ann R. Stavert, Dickon Young, and Matt Rigby
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Daniel Say, Alistair J. Manning, Luke M. Western, Dickon Young, Adam Wisher, Matthew Rigby, Stefan Reimann, Martin K. Vollmer, Michela Maione, Jgor Arduini, Paul B. Krummel, Jens Mühle, Christina M. Harth, Brendan Evans, Ray F. Weiss, Ronald G. Prinn, and Simon O'Doherty
Atmos. Chem. Phys., 21, 2149–2164, https://doi.org/10.5194/acp-21-2149-2021, https://doi.org/10.5194/acp-21-2149-2021, 2021
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Peter G. Simmonds, Matthew Rigby, Alistair J. Manning, Sunyoung Park, Kieran M. Stanley, Archie McCulloch, Stephan Henne, Francesco Graziosi, Michela Maione, Jgor Arduini, Stefan Reimann, Martin K. Vollmer, Jens Mühle, Simon O'Doherty, Dickon Young, Paul B. Krummel, Paul J. Fraser, Ray F. Weiss, Peter K. Salameh, Christina M. Harth, Mi-Kyung Park, Hyeri Park, Tim Arnold, Chris Rennick, L. Paul Steele, Blagoj Mitrevski, Ray H. J. Wang, and Ronald G. Prinn
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Luke M. Western, Zhe Sha, Matthew Rigby, Anita L. Ganesan, Alistair J. Manning, Kieran M. Stanley, Simon J. O'Doherty, Dickon Young, and Jonathan Rougier
Geosci. Model Dev., 13, 2095–2107, https://doi.org/10.5194/gmd-13-2095-2020, https://doi.org/10.5194/gmd-13-2095-2020, 2020
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Assessments of greenhouse gas emissions using atmospheric measurements and meteorological models, or
top-downmethods, are important to verify national inventories or produce a stand-alone estimate where no inventory exists. We present a novel top-down method to estimate emissions. This approach uses a fast method called an integrated nested Laplacian approximation to estimate how these emissions are correlated with other emissions in different locations and at different times.
Ann R. Stavert, Simon O'Doherty, Kieran Stanley, Dickon Young, Alistair J. Manning, Mark F. Lunt, Christopher Rennick, and Tim Arnold
Atmos. Meas. Tech., 12, 4495–4518, https://doi.org/10.5194/amt-12-4495-2019, https://doi.org/10.5194/amt-12-4495-2019, 2019
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Under the UK GAUGE project, two new greenhouse gas observation sites were established in the 2013/2014 winter at two telecommunications towers. A combination of spectroscopic and chromatographic instrumentation was used to measure CO2, CH4, CO, N2O and SF6. The advantages and disadvantages of two CRDS sample drying strategies, Nafion(R) and empirical water correction, were also examined.
Jens Mühle, Cathy M. Trudinger, Luke M. Western, Matthew Rigby, Martin K. Vollmer, Sunyoung Park, Alistair J. Manning, Daniel Say, Anita Ganesan, L. Paul Steele, Diane J. Ivy, Tim Arnold, Shanlan Li, Andreas Stohl, Christina M. Harth, Peter K. Salameh, Archie McCulloch, Simon O'Doherty, Mi-Kyung Park, Chun Ok Jo, Dickon Young, Kieran M. Stanley, Paul B. Krummel, Blagoj Mitrevski, Ove Hermansen, Chris Lunder, Nikolaos Evangeliou, Bo Yao, Jooil Kim, Benjamin Hmiel, Christo Buizert, Vasilii V. Petrenko, Jgor Arduini, Michela Maione, David M. Etheridge, Eleni Michalopoulou, Mike Czerniak, Jeffrey P. Severinghaus, Stefan Reimann, Peter G. Simmonds, Paul J. Fraser, Ronald G. Prinn, and Ray F. Weiss
Atmos. Chem. Phys., 19, 10335–10359, https://doi.org/10.5194/acp-19-10335-2019, https://doi.org/10.5194/acp-19-10335-2019, 2019
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Daniel Say, Anita L. Ganesan, Mark F. Lunt, Matthew Rigby, Simon O'Doherty, Christina Harth, Alistair J. Manning, Paul B. Krummel, and Stephane Bauguitte
Atmos. Chem. Phys., 19, 9865–9885, https://doi.org/10.5194/acp-19-9865-2019, https://doi.org/10.5194/acp-19-9865-2019, 2019
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Despite its emergence as a global economic power, very little information exists regarding India's halocarbon (CFC, HCFC, HFC and chlorocarbon) emissions. We report atmospheric measurements of these gases from above India, and use them to estimate India's emissions. Our results are consistent with the emissions profile of a developing country, with large emissions of HCFCs, HFCs and chlorocarbons not regulated under the Montreal Protocol, but little evidence for ongoing CFC consumption.
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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Joseph R. Pitt, Grant Allen, Stéphane J.-B. Bauguitte, Martin W. Gallagher, James D. Lee, Will Drysdale, Beth Nelson, Alistair J. Manning, and Paul I. Palmer
Atmos. Chem. Phys., 19, 8931–8945, https://doi.org/10.5194/acp-19-8931-2019, https://doi.org/10.5194/acp-19-8931-2019, 2019
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This paper presents a new method to assess inventory estimates of greenhouse gas and air pollutant emissions for large cities and their surrounding regions. A case study using data sampled by a research aircraft around London was used to test the method. We found that the UK national inventory agrees with our observations for CO but needed lower emissions for CH4 to agree with the measured data. Repeated studies could help determine how these emissions vary on different timescales.
Emily D. White, Matthew Rigby, Mark F. Lunt, T. Luke Smallman, Edward Comyn-Platt, Alistair J. Manning, Anita L. Ganesan, Simon O'Doherty, Ann R. Stavert, Kieran Stanley, Mathew Williams, Peter Levy, Michel Ramonet, Grant L. Forster, Andrew C. Manning, and Paul I. Palmer
Atmos. Chem. Phys., 19, 4345–4365, https://doi.org/10.5194/acp-19-4345-2019, https://doi.org/10.5194/acp-19-4345-2019, 2019
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Understanding carbon dioxide (CO2) fluxes from the terrestrial biosphere on a national scale is important for evaluating land use strategies to mitigate climate change. We estimate emissions of CO2 from the UK biosphere using atmospheric data in a top-down approach. Our findings show that bottom-up estimates from models of biospheric fluxes overestimate the amount of CO2 uptake in summer. This suggests these models wrongly estimate or omit key processes, e.g. land disturbance due to harvest.
Kieran Brophy, Heather Graven, Alistair J. Manning, Emily White, Tim Arnold, Marc L. Fischer, Seongeun Jeong, Xinguang Cui, and Matthew Rigby
Atmos. Chem. Phys., 19, 2991–3006, https://doi.org/10.5194/acp-19-2991-2019, https://doi.org/10.5194/acp-19-2991-2019, 2019
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We investigate potential errors and uncertainties related to the spatial and temporal prior representation of emissions and modelled atmospheric transport for the inversion of California's fossil fuel CO2 emissions. Our results indicate that uncertainties in posterior total state fossil fuel CO2 estimates arising from the choice of prior emissions or atmospheric transport model are on the order of 15 % or less for the ground-based network in California we consider.
Daniel Say, Anita L. Ganesan, Mark F. Lunt, Matthew Rigby, Simon O'Doherty, Chris Harth, Alistair J. Manning, Paul B. Krummel, and Stephane Bauguitte
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-1287, https://doi.org/10.5194/acp-2018-1287, 2019
Publication in ACP not foreseen
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India is a potentially significant source of chlorocarbons, gases typically used as solvents and feedstocks. Given the potential for these species to deplete stratospheric ozone, understanding their sources is important. We use flask measurements collected from an aircraft to infer India's chlorocarbon emissions. We link emissions of carbon tetrachloride to the industrial production of other chloromethanes, and provide evidence for rapid growth in India's emissions of dichloromethane.
Sarah Connors, Alistair J. Manning, Andrew D. Robinson, Stuart N. Riddick, Grant L. Forster, Anita Ganesan, Aoife Grant, Stephen Humphrey, Simon O'Doherty, Dave E. Oram, Paul I. Palmer, Robert L. Skelton, Kieran Stanley, Ann Stavert, Dickon Young, and Neil R. P. Harris
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-1187, https://doi.org/10.5194/acp-2018-1187, 2018
Preprint withdrawn
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Methane is an important greenhouse gas & reducing its emissions is a vital part of climate change mitigation to limit global temperature increase to 1.5 °C or 2.0 °C. This paper explains a way to estimate emitted methane over a sub-national area by combining measurements & computer dispersion modelling in a so-called
inversiontechnique. Compared with the current national inventory, our results show lower emissions for Cambridgeshire, possibly due to waste sector emission differences.
Tim Arnold, Alistair J. Manning, Jooil Kim, Shanlan Li, Helen Webster, David Thomson, Jens Mühle, Ray F. Weiss, Sunyoung Park, and Simon O'Doherty
Atmos. Chem. Phys., 18, 13305–13320, https://doi.org/10.5194/acp-18-13305-2018, https://doi.org/10.5194/acp-18-13305-2018, 2018
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Emissions of carbon tetrafluoride CF4, NF3 and CHF3 in east Asia have been calculated using atmospheric measurements and an atmospheric transport model. We calculate emissions of CF4 to be quite constant between the years 2008 and 2015 for both China and South Korea, with 2015 emissions calculated at 4.33 ± 2.65 Gg yr-1 and 0.36 ± 0.11 Gg yr-1, respectively. Emission estimates of NF3 from South Korea could be made with relatively small uncertainty at 0.6 ± 0.07 Gg yr-1 in 2015.
Paul I. Palmer, Simon O'Doherty, Grant Allen, Keith Bower, Hartmut Bösch, Martyn P. Chipperfield, Sarah Connors, Sandip Dhomse, Liang Feng, Douglas P. Finch, Martin W. Gallagher, Emanuel Gloor, Siegfried Gonzi, Neil R. P. Harris, Carole Helfter, Neil Humpage, Brian Kerridge, Diane Knappett, Roderic L. Jones, Michael Le Breton, Mark F. Lunt, Alistair J. Manning, Stephan Matthiesen, Jennifer B. A. Muller, Neil Mullinger, Eiko Nemitz, Sebastian O'Shea, Robert J. Parker, Carl J. Percival, Joseph Pitt, Stuart N. Riddick, Matthew Rigby, Harjinder Sembhi, Richard Siddans, Robert L. Skelton, Paul Smith, Hannah Sonderfeld, Kieran Stanley, Ann R. Stavert, Angelina Wenger, Emily White, Christopher Wilson, and Dickon Young
Atmos. Chem. Phys., 18, 11753–11777, https://doi.org/10.5194/acp-18-11753-2018, https://doi.org/10.5194/acp-18-11753-2018, 2018
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This paper provides an overview of the Greenhouse gAs Uk and Global Emissions (GAUGE) experiment. GAUGE was designed to quantify nationwide GHG emissions of the UK, bringing together measurements and atmospheric transport models. This novel experiment is the first of its kind. We anticipate it will inform the blueprint for countries that are building a measurement infrastructure in preparation for global stocktakes, which are a key part of the Paris Agreement.
Peter G. Simmonds, Matthew Rigby, Archie McCulloch, Martin K. Vollmer, Stephan Henne, Jens Mühle, Simon O'Doherty, Alistair J. Manning, Paul B. Krummel, Paul J. Fraser, Dickon Young, Ray F. Weiss, Peter K. Salameh, Christina M. Harth, Stefan Reimann, Cathy M. Trudinger, L. Paul Steele, Ray H. J. Wang, Diane J. Ivy, Ronald G. Prinn, Blagoj Mitrevski, and David M. Etheridge
Atmos. Chem. Phys., 18, 4153–4169, https://doi.org/10.5194/acp-18-4153-2018, https://doi.org/10.5194/acp-18-4153-2018, 2018
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Recent measurements of the potent greenhouse gas HFC-23, a by-product of HCFC-22 production, show a 28 % increase in the atmospheric mole fraction from 2009 to 2016. A minimum in the atmospheric abundance of HFC-23 in 2009 was attributed to abatement of HFC-23 emissions by incineration under the Clean Development Mechanism (CDM). Our results indicate that the recent increase in HFC-23 emissions is driven by failure of mitigation under the CDM to keep pace with increased HCFC-22 production.
Kieran M. Stanley, Aoife Grant, Simon O'Doherty, Dickon Young, Alistair J. Manning, Ann R. Stavert, T. Gerard Spain, Peter K. Salameh, Christina M. Harth, Peter G. Simmonds, William T. Sturges, David E. Oram, and Richard G. Derwent
Atmos. Meas. Tech., 11, 1437–1458, https://doi.org/10.5194/amt-11-1437-2018, https://doi.org/10.5194/amt-11-1437-2018, 2018
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.
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.
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 G. Simmonds, Matthew Rigby, Archie McCulloch, Simon O'Doherty, Dickon Young, Jens Mühle, Paul B. Krummel, Paul Steele, Paul J. Fraser, Alistair J. Manning, Ray F. Weiss, Peter K. Salameh, Chris M. Harth, Ray H. J. Wang, and Ronald G. Prinn
Atmos. Chem. Phys., 17, 4641–4655, https://doi.org/10.5194/acp-17-4641-2017, https://doi.org/10.5194/acp-17-4641-2017, 2017
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This paper reports how long-term atmospheric measurements demonstrate that the Montreal Protocol has been effective in controlling production and consumption of the hydrochlorofluorocarbons, a group of industrial chemicals that have detrimental effects on the ozone layer and also contribute to global warming as greenhouse gases and their hydrofluorocarbon substitutes which are also potent greenhouse gases but do not materially affect the ozone layer.
Francesco Graziosi, Jgor Arduini, Paolo Bonasoni, Francesco Furlani, Umberto Giostra, Alistair J. Manning, Archie McCulloch, Simon O'Doherty, Peter G. Simmonds, Stefan Reimann, Martin K. Vollmer, and Michela Maione
Atmos. Chem. Phys., 16, 12849–12859, https://doi.org/10.5194/acp-16-12849-2016, https://doi.org/10.5194/acp-16-12849-2016, 2016
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Carbon tetrachloride is an ozone-depleting greenhouse gas banned under the Montreal Protocol. Measurements of atmospheric levels combined with global transport models indicate that it is still being emitted, in contrast to what is reported. In order to help solve the "mystery of carbon tetrachloride", we estimated European emissions during 2006–2014 using atmospheric observations and models. We identified emission hot spots and showed inconsistencies in national emission declarations.
Mark F. Lunt, Matt Rigby, Anita L. Ganesan, and Alistair J. Manning
Geosci. Model Dev., 9, 3213–3229, https://doi.org/10.5194/gmd-9-3213-2016, https://doi.org/10.5194/gmd-9-3213-2016, 2016
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Bayesian inversions can be used to estimate emissions of gases from atmospheric data. We present an inversion framework that objectively defines the basis functions, which describe regions of emissions. The framework allows for the uncertainty in the choice of basis functions to be propagated through to the posterior emissions distribution in a single-step process, and provides an alternative to using a single set of basis functions.
P. G. Simmonds, M. Rigby, A. J. Manning, M. F. Lunt, S. O'Doherty, A. McCulloch, P. J. Fraser, S. Henne, M. K. Vollmer, J. Mühle, R. F. Weiss, P. K. Salameh, D. Young, S. Reimann, A. Wenger, T. Arnold, C. M. Harth, P. B. Krummel, L. P. Steele, B. L. Dunse, B. R. Miller, C. R. Lunder, O. Hermansen, N. Schmidbauer, T. Saito, Y. Yokouchi, S. Park, S. Li, B. Yao, L. X. Zhou, J. Arduini, M. Maione, R. H. J. Wang, D. Ivy, and R. G. Prinn
Atmos. Chem. Phys., 16, 365–382, https://doi.org/10.5194/acp-16-365-2016, https://doi.org/10.5194/acp-16-365-2016, 2016
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We report regional and global emissions estimates of HFC-152a using high frequency measurements from 11 observing sites and archived air samples dating back to 1978 together with atmospheric transport models. The "bottom-up" emissions of HFC-152a reported to the UNFCCC appear to significantly underestimate those reported here from observations. This discrepancy we suggest arises from largely underestimated USA and undeclared Asian emissions.
A. L. Ganesan, A. J. Manning, A. Grant, D. Young, D .E. Oram, W. T. Sturges, J. B. Moncrieff, and S. O'Doherty
Atmos. Chem. Phys., 15, 6393–6406, https://doi.org/10.5194/acp-15-6393-2015, https://doi.org/10.5194/acp-15-6393-2015, 2015
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The UK is one of several countries to enact legislation to reduce its greenhouse gas emissions. We present top-down emissions of methane and nitrous oxide for the UK and Ireland over 2012-2014. We inferred average UK emissions of 2.09Tg/yr CH4 and 0.101Tg/yr N2O and used sectoral distributions to determine whether these discrepancies can be attributed to specific source sectors. We found the agricultural sector likely to be overestimated in the bottom-up emissions inventories of both gases.
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.
S. O'Doherty, M. Rigby, J. Mühle, D. J. Ivy, B. R. Miller, D. Young, P. G. Simmonds, S. Reimann, M. K. Vollmer, P. B. Krummel, P. J. Fraser, L. P. Steele, B. Dunse, P. K. Salameh, C. M. Harth, T. Arnold, R. F. Weiss, J. Kim, S. Park, S. Li, C. Lunder, O. Hermansen, N. Schmidbauer, L. X. Zhou, B. Yao, R. H. J. Wang, A. J. Manning, and R. G. Prinn
Atmos. Chem. Phys., 14, 9249–9258, https://doi.org/10.5194/acp-14-9249-2014, https://doi.org/10.5194/acp-14-9249-2014, 2014
A. L. Ganesan, M. Rigby, A. Zammit-Mangion, A. J. Manning, R. G. Prinn, P. J. Fraser, C. M. Harth, K.-R. Kim, P. B. Krummel, S. Li, J. Mühle, S. J. O'Doherty, S. Park, P. K. Salameh, L. P. Steele, and R. F. Weiss
Atmos. Chem. Phys., 14, 3855–3864, https://doi.org/10.5194/acp-14-3855-2014, https://doi.org/10.5194/acp-14-3855-2014, 2014
M. J. Ashfold, N. R. P. Harris, A. J. Manning, A. D. Robinson, N. J. Warwick, and J. A. Pyle
Atmos. Chem. Phys., 14, 979–994, https://doi.org/10.5194/acp-14-979-2014, https://doi.org/10.5194/acp-14-979-2014, 2014
Markus Jesswein, Valentin Lauther, Nicolas Emig, Peter Hoor, Timo Keber, Hans-Christoph Lachnitt, Linda Ort, Tanja Schuck, Johannes Strobel, Ronja Van Luijt, C. Michael Volk, Franziska Weyland, and Andreas Engel
Atmos. Chem. Phys., 25, 8107–8126, https://doi.org/10.5194/acp-25-8107-2025, https://doi.org/10.5194/acp-25-8107-2025, 2025
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The study investigates transport within the Asian Summer Monsoon, focusing on how CH2Cl2 reaches the subarctic tropopause region. Using data from the PHILEAS campaign in 2023, events with increased mixing ratios were detected. Their origin, the transport paths to the tropopause region, and the potential entry into the stratosphere were analyzed. The East Asian Summer Monsoon was identified as the main transport pathway, with only a small contribution to the stratosphere in the following days.
Luke M. Western, Stephen Bourguet, Molly Crotwell, Lei Hu, Paul B. Krummel, Hélène De Longueville, Alistair J. Mainning, Jens Mühle, Dominique Rust, Isaac Vimont, Martin K. Vollmer, Minde An, Jgor Arduini, Andreas Engel, Paul J. Fraser, Anita L. Ganesan, Christina M. Harth, Chris Lunder, Michela Maione, Stephen A. Montzka, David Nance, Simon O’Doherty, Sunyoung Park, Stefan Reimann, Peter K. Salameh, Roland Schmidt, Kieran M. Stanley, Thomas Wagenhäuser, Dickon Young, Matt Rigby, Ronald G. Prinn, and Ray F. Weiss
EGUsphere, https://doi.org/10.5194/egusphere-2025-3000, https://doi.org/10.5194/egusphere-2025-3000, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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We used atmospheric measurements to estimate emissions of two gases, called HCFC-123 and HCFC-124, that harm the ozone layer. Despite international regulation to stop their production, we found that their emissions have not fallen. This may be linked to how they are used to make other chemicals. Our findings show that some banned substances are still reaching the atmosphere, likely through leaks during chemical production, which could slow the recovery of the ozone layer.
Johannes Degen, Bianca C. Baier, Patrick Jöckel, J. Moritz Menken, Tanja J. Schuck, Colm Sweeney, and Andreas Engel
EGUsphere, https://doi.org/10.5194/egusphere-2025-2648, https://doi.org/10.5194/egusphere-2025-2648, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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We investigate the distribution of CO2 in the upper troposphere and lower stratosphere using both, observations and an atmospheric model. Simulating an artificial tracer, we separate CO2 seasonality from long-term trend and transport variability. We found that patterns in the seasonal signal are attributable to large-scale transport features like the subtropical jet or the Brewer-Dobson circulation. Being a powerful diagnostic tool we recommend to use this tracer for model intercomparisons.
Stephan Henne, Florian R. Storck, Henry Wöhrnschimmel, Markus Leuenberger, Martin K. Vollmer, and Stefan Reimann
EGUsphere, https://doi.org/10.5194/egusphere-2025-2861, https://doi.org/10.5194/egusphere-2025-2861, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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We observed the persistent, man-made trifluoroacetate (TFA) in precipitation and surface waters. Atmospheric simulations attributed TFA to precursor gases in the atmosphere. Although recently increasing concentrations could be followed, gaps in the budget indicate limited understanding of the atmospheric degradation of widely used fluorocarbons. Without additional regulation, environmental TFA concentrations are expected to rise strongly, necessitating continued monitoring and risk assessment.
Luke M. Western, Matthew Rigby, Jens Mühle, Paul B. Krummel, Chris R. Lunder, Simon O'Doherty, Stefan Reimann, Martin K. Vollmer, Dickon Young, Ben Adam, Paul J. Fraser, Anita L. Ganesan, Christina M. Harth, Ove Hermansen, Jooil Kim, Ray L. Langenfelds, Zoë M. Loh, Blagoj Mitrevski, Joseph R. Pitt, Peter K. Salameh, Roland Schmidt, Kieran Stanley, Ann R. Stavert, Hsiang-Jui Wang, Ray F. Weiss, and Ronald G. Prinn
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2025-348, https://doi.org/10.5194/essd-2025-348, 2025
Preprint under review for ESSD
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We used global measurements and an atmospheric model to estimate how emissions and abundances of 42 chemically and radiatively important trace gases have changed over time. These gases affect the Earth's radiative balance and the ozone layer. Our data sets help track progress in reducing harmful. This work supports international efforts to protect the environment by providing clear, long-term, consistent data on how these gases are changing in the atmosphere.
Piers M. Forster, Chris Smith, Tristram Walsh, William F. Lamb, Robin Lamboll, Christophe Cassou, Mathias Hauser, Zeke Hausfather, June-Yi Lee, Matthew D. Palmer, Karina von Schuckmann, Aimée B. A. Slangen, Sophie Szopa, Blair Trewin, Jeongeun Yun, Nathan P. Gillett, Stuart Jenkins, H. Damon Matthews, Krishnan Raghavan, Aurélien Ribes, Joeri Rogelj, Debbie Rosen, Xuebin Zhang, Myles Allen, Lara Aleluia Reis, Robbie M. Andrew, Richard A. Betts, Alex Borger, Jiddu A. Broersma, Samantha N. Burgess, Lijing Cheng, Pierre Friedlingstein, Catia M. Domingues, Marco Gambarini, Thomas Gasser, Johannes Gütschow, Masayoshi Ishii, Christopher Kadow, John Kennedy, Rachel E. Killick, Paul B. Krummel, Aurélien Liné, Didier P. Monselesan, Colin Morice, Jens Mühle, Vaishali Naik, Glen P. Peters, Anna Pirani, Julia Pongratz, Jan C. Minx, Matthew Rigby, Robert Rohde, Abhishek Savita, Sonia I. Seneviratne, Peter Thorne, Christopher Wells, Luke M. Western, Guido R. van der Werf, Susan E. Wijffels, Valérie Masson-Delmotte, and Panmao Zhai
Earth Syst. Sci. Data, 17, 2641–2680, https://doi.org/10.5194/essd-17-2641-2025, https://doi.org/10.5194/essd-17-2641-2025, 2025
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In a rapidly changing climate, evidence-based decision-making benefits from up-to-date and timely information. Here we compile monitoring datasets to track real-world changes over time. To make our work relevant to policymakers, we follow methods from the Intergovernmental Panel on Climate Change (IPCC). Human activities are increasing the Earth's energy imbalance and driving faster sea-level rise compared to the IPCC assessment.
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.
Gerald Wetzel, Anne Kleinert, Sören Johansson, Felix Friedl-Vallon, Michael Höpfner, Jörn Ungermann, Tom Neubert, Valéry Catoire, Cyril Crevoisier, Andreas Engel, Thomas Gulde, Patrick Jacquet, Oliver Kirner, Erik Kretschmer, Thomas Kulessa, Johannes C. Laube, Guido Maucher, Hans Nordmeyer, Christof Piesch, Peter Preusse, Markus Retzlaff, Georg Schardt, Johan Schillings, Herbert Schneider, Axel Schönfeld, Tanja Schuck, Wolfgang Woiwode, Martin Riese, and Peter Braesicke
EGUsphere, https://doi.org/10.5194/egusphere-2025-1838, https://doi.org/10.5194/egusphere-2025-1838, 2025
This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
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We present vertical trace gas profiles from the first balloon flight of the newly developed GLORIA-B limb-imaging Fourier-Transform spectrometer. Longer-lived gases are compared to external measurements to assess the quality of the GLORIA-B observations. Diurnal changes of photochemically active species are compared to model simulations. GLORIA-B demonstrates the capability of balloon-borne limb imaging to provide high-resolution vertical profiles of trace gases up to the middle stratosphere.
Marielle Saunois, Adrien Martinez, Benjamin Poulter, Zhen Zhang, Peter A. Raymond, Pierre Regnier, Josep G. Canadell, Robert B. Jackson, Prabir K. Patra, Philippe Bousquet, Philippe Ciais, Edward J. Dlugokencky, Xin Lan, George H. Allen, David Bastviken, David J. Beerling, Dmitry A. Belikov, Donald R. Blake, Simona Castaldi, Monica Crippa, Bridget R. Deemer, Fraser Dennison, Giuseppe Etiope, Nicola Gedney, Lena Höglund-Isaksson, Meredith A. Holgerson, Peter O. Hopcroft, Gustaf Hugelius, Akihiko Ito, Atul K. Jain, Rajesh Janardanan, Matthew S. Johnson, Thomas Kleinen, Paul B. Krummel, Ronny Lauerwald, Tingting Li, Xiangyu Liu, Kyle C. McDonald, Joe R. Melton, Jens Mühle, Jurek Müller, Fabiola Murguia-Flores, Yosuke Niwa, Sergio Noce, Shufen Pan, Robert J. Parker, Changhui Peng, Michel Ramonet, William J. Riley, Gerard Rocher-Ros, Judith A. Rosentreter, Motoki Sasakawa, Arjo Segers, Steven J. Smith, Emily H. Stanley, Joël Thanwerdas, Hanqin Tian, Aki Tsuruta, Francesco N. Tubiello, Thomas S. Weber, Guido R. van der Werf, Douglas E. J. Worthy, Yi Xi, Yukio Yoshida, Wenxin Zhang, Bo Zheng, Qing Zhu, Qiuan Zhu, and Qianlai Zhuang
Earth Syst. Sci. Data, 17, 1873–1958, https://doi.org/10.5194/essd-17-1873-2025, https://doi.org/10.5194/essd-17-1873-2025, 2025
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Methane (CH4) is the second most important human-influenced greenhouse gas in terms of climate forcing after carbon dioxide (CO2). A consortium of multi-disciplinary scientists synthesise and update the budget of the sources and sinks of CH4. This edition benefits from important progress in estimating emissions from lakes and ponds, reservoirs, and streams and rivers. For the 2010s decade, global CH4 emissions are estimated at 575 Tg CH4 yr-1, including ~65 % from anthropogenic sources.
Timur Cinay, Dickon Young, Nazaret Narváez Jimenez, Cristina Vintimilla-Palacios, Ariel Pila Alonso, Paul B. Krummel, William Vizuete, and Andrew R. Babbin
Atmos. Chem. Phys., 25, 4703–4718, https://doi.org/10.5194/acp-25-4703-2025, https://doi.org/10.5194/acp-25-4703-2025, 2025
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We present the initial 15 months of nitrous oxide measurements from the Galapagos Emissions Monitoring Station. The observed variability in atmospheric mole fractions during this period can be linked to several factors: seasonal variations in trade wind speed and direction across the eastern Pacific, differences in the transport history of air masses sampled, and spatiotemporal heterogeneity in regional marine nitrous oxide emissions from the coastal upwelling systems of Peru and Chile.
Sophie Bauchinger, Andreas Engel, Markus Jesswein, Timo Keber, Harald Bönisch, Florian Obersteiner, Andreas Zahn, Nicolas Emig, Peter Hoor, Hans-Christoph Lachnitt, Franziska Weyland, Linda Ort, and Tanja J. Schuck
EGUsphere, https://doi.org/10.5194/egusphere-2025-1589, https://doi.org/10.5194/egusphere-2025-1589, 2025
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We compared different ways to define the upper barrier of the troposphere in the extra-tropics, the “tropopause”. By analysing ozone distributions sorted by different definitions, we found that the traditional temperature-based tropopause works less well than dynamic or tracer-based definitions. We saw the strongest ozone gradients across the tropopause using a higher value of potential vorticity than often used and recommend this value for future studies of exchange processes in this region.
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.
Laura N. Saunders, Kaley A. Walker, Gabriele P. Stiller, Thomas von Clarmann, Florian Haenel, Hella Garny, Harald Bönisch, Chris D. Boone, Ariana E. Castillo, Andreas Engel, Johannes C. Laube, Marianna Linz, Felix Ploeger, David A. Plummer, Eric A. Ray, and Patrick E. Sheese
Atmos. Chem. Phys., 25, 4185–4209, https://doi.org/10.5194/acp-25-4185-2025, https://doi.org/10.5194/acp-25-4185-2025, 2025
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We present a 17-year stratospheric age-of-air dataset derived from ACE-FTS satellite measurements of sulfur hexafluoride. This is the longest continuous, global, and vertically resolved age of air time series available to date. In this paper, we show that this dataset agrees well with age-of-air datasets based on measurements from other instruments. We also present trends in the midlatitude lower stratosphere that indicate changes in the global circulation that are predicted by climate models.
Martin Vojta, Andreas Plach, Rona L. Thompson, Pallav Purohit, Kieran Stanley, Simon O’Doherty, Dickon Young, Joe Pitt, Xin Lan, and Andreas Stohl
EGUsphere, https://doi.org/10.5194/egusphere-2025-1095, https://doi.org/10.5194/egusphere-2025-1095, 2025
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We determine European emissions of the highly potent greenhouse gas sulfur hexafluoride from 2005 to 2021 – focusing on high-emitting countries and the aggregated EU-27 emissions. Emissions declined in most regions, likely due to EU F-gas regulations. However, our results reveal that most studied countries underestimate their emissions in their national reports. Our sensitivity tests highlight the importance of dense observational networks for reliable inversion-based emission estimates.
Tahereh Alinejadtabrizi, Yi Huang, Francisco Lang, Steven Siems, Michael Manton, Luis Ackermann, Melita Keywood, Ruhi Humphries, Paul Krummel, Alastair Williams, and Greg Ayers
Atmos. Chem. Phys., 25, 2631–2648, https://doi.org/10.5194/acp-25-2631-2025, https://doi.org/10.5194/acp-25-2631-2025, 2025
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Clouds over the Southern Ocean are crucial to Earth's energy balance, but understanding the factors that control them is complex. Our research examines how weather patterns affect tiny particles called cloud condensation nuclei (CCN), which influence cloud properties. Using data from Kennaook / Cape Grim, we found that winter air from Antarctica brings cleaner conditions with lower CCN, while summer patterns from Australia transport more particles. Precipitation also helps reduce CCN in winter.
Fabian Maier, Eva Falge, Maksym Gachkivskyi, Stephan Henne, Ute Karstens, Dafina Kikaj, Ingeborg Levin, Alistair Manning, Christian Rödenbeck, and Christoph Gerbig
EGUsphere, https://doi.org/10.5194/egusphere-2025-477, https://doi.org/10.5194/egusphere-2025-477, 2025
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The radioactive noble gas radon (222Rn) is a suitable natural tracer for atmospheric transport and mixing processes that can be used to validate and calibrate atmospheric transport models. However, this requires accurate estimates of the 222Rn flux from the soil into the atmosphere. In our study, we evaluate the reliability of process-based 222Rn flux maps for Europe using a 222Rn inversion. Our inversion results can give some indications on how to improve the process-based 222Rn flux maps.
Maitane Iturrate-Garcia, Thérèse Salameh, Paul Schlauri, Annarita Baldan, Martin K. Vollmer, Evdokia Stratigou, Sebastien Dusanter, Jianrong Li, Stefan Persijn, Anja Claude, Rupert Holzinger, Christophe Sutour, Tatiana Macé, Yasin Elshorbany, Andreas Ackermann, Céline Pascale, and Stefan Reimann
Atmos. Meas. Tech., 18, 371–403, https://doi.org/10.5194/amt-18-371-2025, https://doi.org/10.5194/amt-18-371-2025, 2025
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Accurate and comparable measurements of oxygenated organic compounds (OVOCs) are crucial in assessing tropospheric ozone burdens and trends. However, the monitoring of many OVOCs remains challenging because of their low atmospheric abundance and lack of stable and traceable calibration standards. This paper describes the calibration standards developed for OVOCs at a low amount of substance fractions (<100 nmol mol-1) to transfer traceability of the International System of Units to the field.
Xiansheng Liu, Xun Zhang, Marvin Dufresne, Tao Wang, Lijie Wu, Rosa Lara, Roger Seco, Marta Monge, Ana Maria Yáñez-Serrano, Marie Gohy, Paul Petit, Audrey Chevalier, Marie-Pierre Vagnot, Yann Fortier, Alexia Baudic, Véronique Ghersi, Grégory Gille, Ludovic Lanzi, Valérie Gros, Leïla Simon, Heidi Héllen, Stefan Reimann, Zoé Le Bras, Michelle Jessy Müller, David Beddows, Siqi Hou, Zongbo Shi, Roy M. Harrison, William Bloss, James Dernie, Stéphane Sauvage, Philip K. Hopke, Xiaoli Duan, Taicheng An, Alastair C. Lewis, James R. Hopkins, Eleni Liakakou, Nikolaos Mihalopoulos, Xiaohu Zhang, Andrés Alastuey, Xavier Querol, and Thérèse Salameh
Atmos. Chem. Phys., 25, 625–638, https://doi.org/10.5194/acp-25-625-2025, https://doi.org/10.5194/acp-25-625-2025, 2025
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This study examines BTEX (benzene, toluene, ethylbenzene, xylenes) pollution in urban areas across seven European countries. Analyzing data from 22 monitoring sites, we found traffic and industrial activities significantly impact BTEX levels, with peaks during rush hours. The risk from BTEX exposure remains moderate, especially in high-traffic and industrial zones, highlighting the need for targeted air quality management to protect public health and improve urban air quality.
Dafina Kikaj, Edward Chung, Alan D. Griffiths, Scott D. Chambers, Grant Forster, Angelina Wenger, Penelope Pickers, Chris Rennick, Simon O'Doherty, Joseph Pitt, Kieran Stanley, Dickon Young, Leigh S. Fleming, Karina Adcock, Emmal Safi, and Tim Arnold
Atmos. Meas. Tech., 18, 151–175, https://doi.org/10.5194/amt-18-151-2025, https://doi.org/10.5194/amt-18-151-2025, 2025
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We present a protocol to improve confidence in atmospheric radon measurements, enabling site comparisons and integration with greenhouse gas data. As a natural tracer, radon provides an independent check of transport model performance. This standardized method enhances radon’s use as a metric for model evaluation. Beyond UK observatories, it can support broader networks like ICOS and WMO/GAW, advancing global atmospheric research.
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.
Martin Vojta, Andreas Plach, Saurabh Annadate, Sunyoung Park, Gawon Lee, Pallav Purohit, Florian Lindl, Xin Lan, Jens Mühle, Rona L. Thompson, and Andreas Stohl
Atmos. Chem. Phys., 24, 12465–12493, https://doi.org/10.5194/acp-24-12465-2024, https://doi.org/10.5194/acp-24-12465-2024, 2024
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We constrain the global emissions of the very potent greenhouse gas sulfur hexafluoride (SF6) between 2005 and 2021. We show that SF6 emissions are decreasing in the USA and in the EU, while they are substantially growing in China, leading overall to an increasing global emission trend. The national reports for the USA, EU, and China all underestimated their SF6 emissions. However, stringent mitigation measures can successfully reduce SF6 emissions, as can be seen in the EU emission trend.
Gabrielle Pétron, Andrew M. Crotwell, John Mund, Molly Crotwell, Thomas Mefford, Kirk Thoning, Bradley Hall, Duane Kitzis, Monica Madronich, Eric Moglia, Donald Neff, Sonja Wolter, Armin Jordan, Paul Krummel, Ray Langenfelds, and John Patterson
Atmos. Meas. Tech., 17, 4803–4823, https://doi.org/10.5194/amt-17-4803-2024, https://doi.org/10.5194/amt-17-4803-2024, 2024
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Hydrogen (H2) is a gas in trace amounts in the Earth’s atmosphere with indirect impacts on climate and air quality. Renewed interest in H2 as a low- or zero-carbon source of energy may lead to increased production, uses, and supply chain emissions. NOAA measurements of weekly air samples collected between 2009 and 2021 at over 50 sites in mostly remote locations are now available, and they complement other datasets to study the H2 global budget.
Benjamin Hmiel, Vasilii V. Petrenko, Christo Buizert, Andrew M. Smith, Michael N. Dyonisius, Philip Place, Bin Yang, Quan Hua, Ross Beaudette, Jeffrey P. Severinghaus, Christina Harth, Ray F. Weiss, Lindsey Davidge, Melisa Diaz, Matthew Pacicco, James A. Menking, Michael Kalk, Xavier Faïn, Alden Adolph, Isaac Vimont, and Lee T. Murray
The Cryosphere, 18, 3363–3382, https://doi.org/10.5194/tc-18-3363-2024, https://doi.org/10.5194/tc-18-3363-2024, 2024
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The main aim of this research is to improve understanding of carbon-14 that is produced by cosmic rays in ice sheets. Measurements of carbon-14 in ice cores can provide a range of useful information (age of ice, past atmospheric chemistry, past cosmic ray intensity). Our results show that almost all (>99 %) of carbon-14 that is produced in the upper layer of ice sheets is rapidly lost to the atmosphere. Our results also provide better estimates of carbon-14 production rates in deeper ice.
Yao Ge, Sverre Solberg, Mathew R. Heal, Stefan Reimann, Willem van Caspel, Bryan Hellack, Thérèse Salameh, and David Simpson
Atmos. Chem. Phys., 24, 7699–7729, https://doi.org/10.5194/acp-24-7699-2024, https://doi.org/10.5194/acp-24-7699-2024, 2024
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Atmospheric volatile organic compounds (VOCs) constitute many species, acting as precursors to ozone and aerosol. Given the uncertainties in VOC emissions, lack of evaluation studies, and recent changes in emissions, this work adapts the EMEP MSC-W to evaluate emission inventories in Europe. We focus on the varying agreement between modelled and measured VOCs across different species and underscore potential inaccuracies in total and sector-specific emission estimates.
Haklim Choi, Alison L. Redington, Hyeri Park, Jooil Kim, Rona L. Thompson, Jens Mühle, Peter K. Salameh, Christina M. Harth, Ray F. Weiss, Alistair J. Manning, and Sunyoung Park
Atmos. Chem. Phys., 24, 7309–7330, https://doi.org/10.5194/acp-24-7309-2024, https://doi.org/10.5194/acp-24-7309-2024, 2024
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We analyzed with an inversion model the atmospheric abundance of hydrofluorocarbons (HFCs), potent greenhouse gases, from 2008 to 2020 at Gosan station in South Korea and revealed a significant increase in emissions, especially from eastern China and Japan. This increase contradicts reported data, underscoring the need for accurate monitoring and reporting. Our findings are crucial for understanding and managing global HFCs emissions, highlighting the importance of efforts to reduce HFCs.
Hanqin Tian, Naiqing Pan, Rona L. Thompson, Josep G. Canadell, Parvadha Suntharalingam, Pierre Regnier, Eric A. Davidson, Michael Prather, Philippe Ciais, Marilena Muntean, Shufen Pan, Wilfried Winiwarter, Sönke Zaehle, Feng Zhou, Robert B. Jackson, Hermann W. Bange, Sarah Berthet, Zihao Bian, Daniele Bianchi, Alexander F. Bouwman, Erik T. Buitenhuis, Geoffrey Dutton, Minpeng Hu, Akihiko Ito, Atul K. Jain, Aurich Jeltsch-Thömmes, Fortunat Joos, Sian Kou-Giesbrecht, Paul B. Krummel, Xin Lan, Angela Landolfi, Ronny Lauerwald, Ya Li, Chaoqun Lu, Taylor Maavara, Manfredi Manizza, Dylan B. Millet, Jens Mühle, Prabir K. Patra, Glen P. Peters, Xiaoyu Qin, Peter Raymond, Laure Resplandy, Judith A. Rosentreter, Hao Shi, Qing Sun, Daniele Tonina, Francesco N. Tubiello, Guido R. van der Werf, Nicolas Vuichard, Junjie Wang, Kelley C. Wells, Luke M. Western, Chris Wilson, Jia Yang, Yuanzhi Yao, Yongfa You, and Qing Zhu
Earth Syst. Sci. Data, 16, 2543–2604, https://doi.org/10.5194/essd-16-2543-2024, https://doi.org/10.5194/essd-16-2543-2024, 2024
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Atmospheric concentrations of nitrous oxide (N2O), a greenhouse gas 273 times more potent than carbon dioxide, have increased by 25 % since the preindustrial period, with the highest observed growth rate in 2020 and 2021. This rapid growth rate has primarily been due to a 40 % increase in anthropogenic emissions since 1980. Observed atmospheric N2O concentrations in recent years have exceeded the worst-case climate scenario, underscoring the importance of reducing anthropogenic N2O emissions.
Piers M. Forster, Chris Smith, Tristram Walsh, William F. Lamb, Robin Lamboll, Bradley Hall, Mathias Hauser, Aurélien Ribes, Debbie Rosen, Nathan P. Gillett, Matthew D. Palmer, Joeri Rogelj, Karina von Schuckmann, Blair Trewin, Myles Allen, Robbie Andrew, Richard A. Betts, Alex Borger, Tim Boyer, Jiddu A. Broersma, Carlo Buontempo, Samantha Burgess, Chiara Cagnazzo, Lijing Cheng, Pierre Friedlingstein, Andrew Gettelman, Johannes Gütschow, Masayoshi Ishii, Stuart Jenkins, Xin Lan, Colin Morice, Jens Mühle, Christopher Kadow, John Kennedy, Rachel E. Killick, Paul B. Krummel, Jan C. Minx, Gunnar Myhre, Vaishali Naik, Glen P. Peters, Anna Pirani, Julia Pongratz, Carl-Friedrich Schleussner, Sonia I. Seneviratne, Sophie Szopa, Peter Thorne, Mahesh V. M. Kovilakam, Elisa Majamäki, Jukka-Pekka Jalkanen, Margreet van Marle, Rachel M. Hoesly, Robert Rohde, Dominik Schumacher, Guido van der Werf, Russell Vose, Kirsten Zickfeld, Xuebin Zhang, Valérie Masson-Delmotte, and Panmao Zhai
Earth Syst. Sci. Data, 16, 2625–2658, https://doi.org/10.5194/essd-16-2625-2024, https://doi.org/10.5194/essd-16-2625-2024, 2024
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This paper tracks some key indicators of global warming through time, from 1850 through to the end of 2023. It is designed to give an authoritative estimate of global warming to date and its causes. We find that in 2023, global warming reached 1.3 °C and is increasing at over 0.2 °C per decade. This is caused by all-time-high greenhouse gas emissions.
Felicia Kolonjari, Patrick E. Sheese, Kaley A. Walker, Chris D. Boone, David A. Plummer, Andreas Engel, Stephen A. Montzka, David E. Oram, Tanja Schuck, Gabriele P. Stiller, and Geoffrey C. Toon
Atmos. Meas. Tech., 17, 2429–2449, https://doi.org/10.5194/amt-17-2429-2024, https://doi.org/10.5194/amt-17-2429-2024, 2024
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The Canadian Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS) satellite instrument is currently providing the only vertically resolved chlorodifluoromethane (HCFC-22) measurements from space. This study assesses the most current ACE-FTS HCFC-22 data product in the upper troposphere and lower stratosphere, as well as modelled HCFC-22 from a 39-year run of the Canadian Middle Atmosphere Model (CMAM39) in the same region.
Hannah Chawner, Eric Saboya, Karina E. Adcock, Tim Arnold, Yuri Artioli, Caroline Dylag, Grant L. Forster, Anita Ganesan, Heather Graven, Gennadi Lessin, Peter Levy, Ingrid T. Luijkx, Alistair Manning, Penelope A. Pickers, Chris Rennick, Christian Rödenbeck, and Matthew Rigby
Atmos. Chem. Phys., 24, 4231–4252, https://doi.org/10.5194/acp-24-4231-2024, https://doi.org/10.5194/acp-24-4231-2024, 2024
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The quantity of atmospheric potential oxygen (APO), derived from coincident measurements of carbon dioxide (CO2) and oxygen (O2), has been proposed as a tracer for fossil fuel CO2 emissions. In this model sensitivity study, we examine the use of APO for this purpose in the UK and compare our model to observations. We find that our model simulations are most sensitive to uncertainties relating to ocean fluxes and boundary conditions.
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.
Rona L. Thompson, Stephen A. Montzka, Martin K. Vollmer, Jgor Arduini, Molly Crotwell, Paul B. Krummel, Chris Lunder, Jens Mühle, Simon O'Doherty, Ronald G. Prinn, Stefan Reimann, Isaac Vimont, Hsiang Wang, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 24, 1415–1427, https://doi.org/10.5194/acp-24-1415-2024, https://doi.org/10.5194/acp-24-1415-2024, 2024
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The hydroxyl radical determines the atmospheric lifetimes of numerous species including methane. Since OH is very short-lived, it is not possible to directly measure its concentration on scales relevant for understanding its effect on other species. Here, OH is inferred by looking at changes in hydrofluorocarbons (HFCs). We find that OH levels have been fairly stable over our study period (2004 to 2021), suggesting that OH is not the main driver of the recent increase in atmospheric methane.
Tanja J. Schuck, Johannes Degen, Eric Hintsa, Peter Hoor, Markus Jesswein, Timo Keber, Daniel Kunkel, Fred Moore, Florian Obersteiner, Matt Rigby, Thomas Wagenhäuser, Luke M. Western, Andreas Zahn, and Andreas Engel
Atmos. Chem. Phys., 24, 689–705, https://doi.org/10.5194/acp-24-689-2024, https://doi.org/10.5194/acp-24-689-2024, 2024
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We study the interhemispheric gradient of sulfur hexafluoride (SF6), a strong long-lived greenhouse gas. Its emissions are stronger in the Northern Hemisphere; therefore, mixing ratios in the Southern Hemisphere lag behind. Comparing the observations to a box model, the model predicts air in the Southern Hemisphere to be older. For a better agreement, the emissions used as model input need to be increased (and their spatial pattern changed), and we need to modify north–south transport.
Douglas E. J. Worthy, Michele K. Rauh, Lin Huang, Felix R. Vogel, Alina Chivulescu, Kenneth A. Masarie, Ray L. Langenfelds, Paul B. Krummel, Colin E. Allison, Andrew M. Crotwell, Monica Madronich, Gabrielle Pétron, Ingeborg Levin, Samuel Hammer, Sylvia Michel, Michel Ramonet, Martina Schmidt, Armin Jordan, Heiko Moossen, Michael Rothe, Ralph Keeling, and Eric J. Morgan
Atmos. Meas. Tech., 16, 5909–5935, https://doi.org/10.5194/amt-16-5909-2023, https://doi.org/10.5194/amt-16-5909-2023, 2023
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Network compatibility is important for inferring greenhouse gas fluxes at global or regional scales. This study is the first assessment of the measurement agreement among seven individual programs within the World Meteorological Organization community. It compares co-located flask air measurements at the Alert Observatory in Canada over a 17-year period. The results provide stronger confidence in the uncertainty estimation while using those datasets in various data interpretation applications.
John D. Patterson, Murat Aydin, Andrew M. Crotwell, Gabrielle Pétron, Jeffery P. Severinghaus, Paul B. Krummel, Ray L. Langenfelds, Vasilii V. Petrenko, and Eric S. Saltzman
Clim. Past, 19, 2535–2550, https://doi.org/10.5194/cp-19-2535-2023, https://doi.org/10.5194/cp-19-2535-2023, 2023
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Atmospheric levels of molecular hydrogen (H2) can impact climate and air quality. Constraining past changes to atmospheric H2 is useful for understanding how H2 cycles through the Earth system and predicting the impacts of increasing anthropogenic emissions under the
hydrogen economy. Here, we use the aging air found in the polar snowpack to reconstruct H2 levels over the past 100 years. We find that H2 levels increased by 30 % over Greenland and 60 % over Antarctica during the 20th century.
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.
Hyeri Park, Jooil Kim, Haklim Choi, Sohyeon Geum, Yeaseul Kim, Rona L. Thompson, Jens Mühle, Peter K. Salameh, Christina M. Harth, Kieran M. Stanley, Simon O'Doherty, Paul J. Fraser, Peter G. Simmonds, Paul B. Krummel, Ray F. Weiss, Ronald G. Prinn, and Sunyoung Park
Atmos. Chem. Phys., 23, 9401–9411, https://doi.org/10.5194/acp-23-9401-2023, https://doi.org/10.5194/acp-23-9401-2023, 2023
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Based on atmospheric HFC-23 observations, the first estimate of post-CDM HFC-23 emissions in eastern Asia for 2008–2019 shows that these emissions contribute significantly to the global emissions rise. The observation-derived emissions were much larger than the bottom-up estimates expected to approach zero after 2015 due to national abatement activities. These discrepancies could be attributed to unsuccessful factory-level HFC-23 abatement and inaccurate quantification of emission reductions.
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.
Alice Drinkwater, Paul I. Palmer, Liang Feng, Tim Arnold, Xin Lan, Sylvia E. Michel, Robert Parker, and Hartmut Boesch
Atmos. Chem. Phys., 23, 8429–8452, https://doi.org/10.5194/acp-23-8429-2023, https://doi.org/10.5194/acp-23-8429-2023, 2023
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Changes in atmospheric methane over the last few decades are largely unexplained. Previous studies have proposed different hypotheses to explain short-term changes in atmospheric methane. We interpret observed changes in atmospheric methane and stable isotope source signatures (2004–2020). We argue that changes over this period are part of a large-scale shift from high-northern-latitude thermogenic energy emissions to tropical biogenic emissions, particularly from North Africa and South America.
Alison L. Redington, Alistair J. Manning, Stephan Henne, Francesco Graziosi, Luke M. Western, Jgor Arduini, Anita L. Ganesan, Christina M. Harth, Michela Maione, Jens Mühle, Simon O'Doherty, Joseph Pitt, Stefan Reimann, Matthew Rigby, Peter K. Salameh, Peter G. Simmonds, T. Gerard Spain, Kieran Stanley, Martin K. Vollmer, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 23, 7383–7398, https://doi.org/10.5194/acp-23-7383-2023, https://doi.org/10.5194/acp-23-7383-2023, 2023
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Chlorofluorocarbons (CFCs) were used in Europe pre-1990, damaging the stratospheric ozone layer. Legislation has controlled production and use, and global emissions have decreased sharply. The global rate of decline in CFC-11 recently slowed and was partly attributed to illegal emission in eastern China. This study concludes that emissions of CFC-11 in western Europe have not contributed to the unexplained part of the global increase in CFC-11 observed in the last decade.
Emily Dowd, Chris Wilson, Martyn P. Chipperfield, Emanuel Gloor, Alistair Manning, and Ruth Doherty
Atmos. Chem. Phys., 23, 7363–7382, https://doi.org/10.5194/acp-23-7363-2023, https://doi.org/10.5194/acp-23-7363-2023, 2023
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Surface observations of methane show that the seasonal cycle amplitude (SCA) of methane is decreasing in the northern high latitudes (NHLs) but increased globally (1995–2020). The NHL decrease is counterintuitive, as we expect the SCA to increase with increasing concentrations. We use a chemical transport model to investigate changes in SCA in the NHLs. We find well-mixed methane and changes in emissions from Canada, the Middle East, and Europe are the largest contributors to the SCA in NHLs.
Elena Fillola, Raul Santos-Rodriguez, Alistair Manning, Simon O'Doherty, and Matt Rigby
Geosci. Model Dev., 16, 1997–2009, https://doi.org/10.5194/gmd-16-1997-2023, https://doi.org/10.5194/gmd-16-1997-2023, 2023
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Lagrangian particle dispersion models are used extensively for the estimation of greenhouse gas (GHG) fluxes using atmospheric observations. However, these models do not scale well as data volumes increase. Here, we develop a proof-of-concept machine learning emulator that can produce outputs similar to those of the dispersion model, but 50 000 times faster, using only meteorological inputs. This works demonstrates the potential of machine learning to accelerate GHG estimations across the globe.
Thomas Wagenhäuser, Markus Jesswein, Timo Keber, Tanja Schuck, and Andreas Engel
Atmos. Chem. Phys., 23, 3887–3903, https://doi.org/10.5194/acp-23-3887-2023, https://doi.org/10.5194/acp-23-3887-2023, 2023
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A common assumption to derive mean age from trace gas observations is that all air enters the stratosphere through the tropical tropopause. Using SF6 as an age tracer, this leads to negative mean age values close to the Northern Hemispheric extra-tropical tropopause. Our improved method also considers extra-tropical input into the stratosphere. More realistic values are derived using this method. Interhemispheric differences in mean age are found when comparing data from two aircraft campaigns.
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.
Michael N. Dyonisius, Vasilii V. Petrenko, Andrew M. Smith, Benjamin Hmiel, Peter D. Neff, Bin Yang, Quan Hua, Jochen Schmitt, Sarah A. Shackleton, Christo Buizert, Philip F. Place, James A. Menking, Ross Beaudette, Christina Harth, Michael Kalk, Heidi A. Roop, Bernhard Bereiter, Casey Armanetti, Isaac Vimont, Sylvia Englund Michel, Edward J. Brook, Jeffrey P. Severinghaus, Ray F. Weiss, and Joseph R. McConnell
The Cryosphere, 17, 843–863, https://doi.org/10.5194/tc-17-843-2023, https://doi.org/10.5194/tc-17-843-2023, 2023
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Cosmic rays that enter the atmosphere produce secondary particles which react with surface minerals to produce radioactive nuclides. These nuclides are often used to constrain Earth's surface processes. However, the production rates from muons are not well constrained. We measured 14C in ice with a well-known exposure history to constrain the production rates from muons. 14C production in ice is analogous to quartz, but we obtain different production rates compared to commonly used estimates.
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.
Markus Jesswein, Rafael P. Fernandez, Lucas Berná, Alfonso Saiz-Lopez, Jens-Uwe Grooß, Ryan Hossaini, Eric C. Apel, Rebecca S. Hornbrook, Elliot L. Atlas, Donald R. Blake, Stephen Montzka, Timo Keber, Tanja Schuck, Thomas Wagenhäuser, and Andreas Engel
Atmos. Chem. Phys., 22, 15049–15070, https://doi.org/10.5194/acp-22-15049-2022, https://doi.org/10.5194/acp-22-15049-2022, 2022
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This study presents the global and seasonal distribution of the two major brominated short-lived substances CH2Br2 and CHBr3 in the upper troposphere and lower stratosphere based on observations from several aircraft campaigns. They show similar seasonality for both hemispheres, except in the respective hemispheric autumn lower stratosphere. A comparison with the TOMCAT and CAM-Chem models shows good agreement in the annual mean but larger differences in the seasonal consideration.
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.
Angharad C. Stell, Michael Bertolacci, Andrew Zammit-Mangion, Matthew Rigby, Paul J. Fraser, Christina M. Harth, Paul B. Krummel, Xin Lan, Manfredi Manizza, Jens Mühle, Simon O'Doherty, Ronald G. Prinn, Ray F. Weiss, Dickon Young, and Anita L. Ganesan
Atmos. Chem. Phys., 22, 12945–12960, https://doi.org/10.5194/acp-22-12945-2022, https://doi.org/10.5194/acp-22-12945-2022, 2022
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Nitrous oxide is a potent greenhouse gas and ozone-depleting substance, whose atmospheric abundance has risen throughout the contemporary record. In this work, we carry out the first global hierarchical Bayesian inversion to solve for nitrous oxide emissions. We derive increasing global nitrous oxide emissions over 2011–2020, which are mainly driven by emissions between 0° and 30°N, with the highest emissions recorded in 2020.
Maria Paula Pérez-Peña, Jenny A. Fisher, Dylan B. Millet, Hisashi Yashiro, Ray L. Langenfelds, Paul B. Krummel, and Scott H. Kable
Atmos. Chem. Phys., 22, 12367–12386, https://doi.org/10.5194/acp-22-12367-2022, https://doi.org/10.5194/acp-22-12367-2022, 2022
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We used two atmospheric models to test the implications of previously unexplored aldehyde photochemistry on the atmospheric levels of molecular hydrogen (H2). We showed that the new photochemistry from aldehydes produces more H2 over densely forested areas. Compared to the rest of the world, it is over these forested regions where the produced H2 is more likely to be removed. The results highlight that other processes that contribute to atmospheric H2 levels should be studied further.
Megan Jeramaz Lickley, John S. Daniel, Eric L. Fleming, Stefan Reimann, and Susan Solomon
Atmos. Chem. Phys., 22, 11125–11136, https://doi.org/10.5194/acp-22-11125-2022, https://doi.org/10.5194/acp-22-11125-2022, 2022
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Halocarbons contained in equipment continue to be emitted after production has ceased. These
banksmust be carefully accounted for in evaluating compliance with the Montreal Protocol. We extend a Bayesian model to the suite of regulated chemicals subject to banking. We find that banks are substantially larger than previous estimates, and we identify banks by chemical and equipment type whose future emissions will contribute to global warming and delay ozone-hole recovery if left unrecovered.
Luke M. Western, Alison L. Redington, Alistair J. Manning, Cathy M. Trudinger, Lei Hu, Stephan Henne, Xuekun Fang, Lambert J. M. Kuijpers, Christina Theodoridi, David S. Godwin, Jgor Arduini, Bronwyn Dunse, Andreas Engel, Paul J. Fraser, Christina M. Harth, Paul B. Krummel, Michela Maione, Jens Mühle, Simon O'Doherty, Hyeri Park, Sunyoung Park, Stefan Reimann, Peter K. Salameh, Daniel Say, Roland Schmidt, Tanja Schuck, Carolina Siso, Kieran M. Stanley, Isaac Vimont, Martin K. Vollmer, Dickon Young, Ronald G. Prinn, Ray F. Weiss, Stephen A. Montzka, and Matthew Rigby
Atmos. Chem. Phys., 22, 9601–9616, https://doi.org/10.5194/acp-22-9601-2022, https://doi.org/10.5194/acp-22-9601-2022, 2022
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The production of ozone-destroying gases is being phased out. Even though production of one of the main ozone-depleting gases, called HCFC-141b, has been declining for many years, the amount that is being released to the atmosphere has been increasing since 2017. We do not know for sure why this is. A possible explanation is that HCFC-141b that was used to make insulating foams many years ago is only now escaping to the atmosphere, or a large part of its production is not being reported.
Guus J. M. Velders, John S. Daniel, Stephen A. Montzka, Isaac Vimont, Matthew Rigby, Paul B. Krummel, Jens Muhle, Simon O'Doherty, Ronald G. Prinn, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 22, 6087–6101, https://doi.org/10.5194/acp-22-6087-2022, https://doi.org/10.5194/acp-22-6087-2022, 2022
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The emissions of hydrofluorocarbons (HFCs) have increased significantly in the past as a result of the phasing out of ozone-depleting substances. Observations indicate that HFCs are used much less in certain refrigeration applications than previously projected. Current policies are projected to reduce emissions and the surface temperature contribution of HFCs from 0.28–0.44 °C to 0.14–0.31 °C in 2100. The Kigali Amendment is projected to reduce the contributions further to 0.04 °C in 2100.
Haklim Choi, Mi-Kyung Park, Paul J. Fraser, Hyeri Park, Sohyeon Geum, Jens Mühle, Jooil Kim, Ian Porter, Peter K. Salameh, Christina M. Harth, Bronwyn L. Dunse, Paul B. Krummel, Ray F. Weiss, Simon O'Doherty, Dickon Young, and Sunyoung Park
Atmos. Chem. Phys., 22, 5157–5173, https://doi.org/10.5194/acp-22-5157-2022, https://doi.org/10.5194/acp-22-5157-2022, 2022
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We observed 12-year continuous CH3Br pollution signals at Gosan and estimated anthropogenic CH3Br emissions in eastern China. The analysis revealed a significant discrepancy between top-down estimates and the bottom-up emissions from the fumigation usage reported to the United Nations Environment Programme, likely due to unreported or inaccurately reported fumigation usage. This result provides information to monitor international compliance with the Montreal Protocol.
Alice E. Ramsden, Anita L. Ganesan, Luke M. Western, Matthew Rigby, Alistair J. Manning, Amy Foulds, James L. France, Patrick Barker, Peter Levy, Daniel Say, Adam Wisher, Tim Arnold, Chris Rennick, Kieran M. Stanley, Dickon Young, and Simon O'Doherty
Atmos. Chem. Phys., 22, 3911–3929, https://doi.org/10.5194/acp-22-3911-2022, https://doi.org/10.5194/acp-22-3911-2022, 2022
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Quantifying methane emissions from different sources is a key focus of current research. We present a method for estimating sectoral methane emissions that uses ethane as a tracer for fossil fuel methane. By incorporating variable ethane : methane emission ratios into this model, we produce emissions estimates with improved uncertainty characterisation. This method will be particularly useful for studying methane emissions in areas with complex distributions of sources.
Danilo Custódio, Katrine Aspmo Pfaffhuber, T. Gerard Spain, Fidel F. Pankratov, Iana Strigunova, Koketso Molepo, Henrik Skov, Johannes Bieser, and Ralf Ebinghaus
Atmos. Chem. Phys., 22, 3827–3840, https://doi.org/10.5194/acp-22-3827-2022, https://doi.org/10.5194/acp-22-3827-2022, 2022
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As a poison in the air that we breathe and the food that we eat, mercury is a human health concern for society as a whole. In that regard, this work deals with monitoring and modelling mercury in the environment, improving wherewithal, identifying the strength of the different components at play, and interpreting information to support the efforts that seek to safeguard public health.
Peter Sperlich, Gordon W. Brailsford, Rowena C. Moss, John McGregor, Ross J. Martin, Sylvia Nichol, Sara Mikaloff-Fletcher, Beata Bukosa, Magda Mandic, C. Ian Schipper, Paul Krummel, and Alan D. Griffiths
Atmos. Meas. Tech., 15, 1631–1656, https://doi.org/10.5194/amt-15-1631-2022, https://doi.org/10.5194/amt-15-1631-2022, 2022
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We tested an in situ analyser for carbon and oxygen isotopes in atmospheric CO2 at Baring Head, New Zealand’s observatory for Southern Ocean baseline air. The analyser was able to resolve regional signals of the terrestrial carbon cycle, although the analysis of small events was limited by analytical uncertainty. Further improvement of the instrument performance would be desirable for the robust analysis of distant signals and to resolve the small variability in Southern Ocean baseline air.
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.
Helmut Ziereis, Peter Hoor, Jens-Uwe Grooß, Andreas Zahn, Greta Stratmann, Paul Stock, Michael Lichtenstern, Jens Krause, Vera Bense, Armin Afchine, Christian Rolf, Wolfgang Woiwode, Marleen Braun, Jörn Ungermann, Andreas Marsing, Christiane Voigt, Andreas Engel, Björn-Martin Sinnhuber, and Hermann Oelhaf
Atmos. Chem. Phys., 22, 3631–3654, https://doi.org/10.5194/acp-22-3631-2022, https://doi.org/10.5194/acp-22-3631-2022, 2022
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Airborne observations were conducted in the lowermost Arctic stratosphere during the winter of 2015/2016. The observed distribution of reactive nitrogen shows clear indications of nitrification in mid-winter and denitrification in late winter. This was caused by the formation of polar stratospheric cloud particles, which were observed during several flights. The sedimentation and evaporation of these particles and the descent of air masses cause a redistribution of reactive nitrogen.
Jens Mühle, Lambert J. M. Kuijpers, Kieran M. Stanley, Matthew Rigby, Luke M. Western, Jooil Kim, Sunyoung Park, Christina M. Harth, Paul B. Krummel, Paul J. Fraser, Simon O'Doherty, Peter K. Salameh, Roland Schmidt, Dickon Young, Ronald G. Prinn, Ray H. J. Wang, and Ray F. Weiss
Atmos. Chem. Phys., 22, 3371–3378, https://doi.org/10.5194/acp-22-3371-2022, https://doi.org/10.5194/acp-22-3371-2022, 2022
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Emissions of the strong greenhouse gas perfluorocyclobutane (c-C4F8) into the atmosphere have been increasing sharply since the early 2000s. These c-C4F8 emissions are highly correlated with the amount of hydrochlorofluorocarbon-22 produced to synthesize polytetrafluoroethylene (known for its non-stick properties) and related chemicals. From this process, c-C4F8 by-product is vented to the atmosphere. Avoiding these unnecessary c-C4F8 emissions could reduce the climate impact of this industry.
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.
Markus Jesswein, Heiko Bozem, Hans-Christoph Lachnitt, Peter Hoor, Thomas Wagenhäuser, Timo Keber, Tanja Schuck, and Andreas Engel
Atmos. Chem. Phys., 21, 17225–17241, https://doi.org/10.5194/acp-21-17225-2021, https://doi.org/10.5194/acp-21-17225-2021, 2021
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This study presents and compares inorganic chlorine (Cly) derived from observations with the HALO research aircraft in the Antarctic late winter–early fall 2019 and the Arctic winter 2015–2016. Trend-corrected correlations from the Northern Hemisphere show excellent agreement with those from the Southern Hemisphere. After observation allocation inside and outside the vortex based on N2O measurements, results of the two campaigns reveal substantial differences in Cly within the respective vortex.
Paul D. Hamer, Virginie Marécal, Ryan Hossaini, Michel Pirre, Gisèle Krysztofiak, Franziska Ziska, Andreas Engel, Stephan Sala, Timo Keber, Harald Bönisch, Elliot Atlas, Kirstin Krüger, Martyn Chipperfield, Valery Catoire, Azizan A. Samah, Marcel Dorf, Phang Siew Moi, Hans Schlager, and Klaus Pfeilsticker
Atmos. Chem. Phys., 21, 16955–16984, https://doi.org/10.5194/acp-21-16955-2021, https://doi.org/10.5194/acp-21-16955-2021, 2021
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Bromoform is a stratospheric ozone-depleting gas released by seaweed and plankton transported to the stratosphere via convection in the tropics. We study the chemical interactions of bromoform and its derivatives within convective clouds using a cloud-scale model and observations. Our findings are that soluble bromine gases are efficiently washed out and removed within the convective clouds and that most bromine is transported vertically to the upper troposphere in the form of bromoform.
Mark F. Lunt, Alistair J. Manning, Grant Allen, Tim Arnold, Stéphane J.-B. Bauguitte, Hartmut Boesch, Anita L. Ganesan, Aoife Grant, Carole Helfter, Eiko Nemitz, Simon J. O'Doherty, Paul I. Palmer, Joseph R. Pitt, Chris Rennick, Daniel Say, Kieran M. Stanley, Ann R. Stavert, Dickon Young, and Matt Rigby
Atmos. Chem. Phys., 21, 16257–16276, https://doi.org/10.5194/acp-21-16257-2021, https://doi.org/10.5194/acp-21-16257-2021, 2021
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We present an evaluation of the UK's methane emissions between 2013 and 2020 using a network of tall tower measurement sites. We find emissions that are consistent in both magnitude and trend with the UK's reported emissions, with a declining trend driven by a decrease in emissions from England. The impact of various components of the modelling set-up on these findings are explored through a number of sensitivity studies.
Meike K. Rotermund, Vera Bense, Martyn P. Chipperfield, Andreas Engel, Jens-Uwe Grooß, Peter Hoor, Tilman Hüneke, Timo Keber, Flora Kluge, Benjamin Schreiner, Tanja Schuck, Bärbel Vogel, Andreas Zahn, and Klaus Pfeilsticker
Atmos. Chem. Phys., 21, 15375–15407, https://doi.org/10.5194/acp-21-15375-2021, https://doi.org/10.5194/acp-21-15375-2021, 2021
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Airborne total bromine (Brtot) and tracer measurements suggest Brtot-rich air masses persistently protruded into the lower stratosphere (LS), creating a high Brtot region over the North Atlantic in fall 2017. The main source is via isentropic transport by the Asian monsoon and to a lesser extent transport across the extratropical tropopause as quantified by a Lagrange model. The transport of Brtot via Central American hurricanes is also observed. Lastly, the impact of Brtot on LS O3 is assessed.
Masanori Takeda, Hideaki Nakajima, Isao Murata, Tomoo Nagahama, Isamu Morino, Geoffrey C. Toon, Ray F. Weiss, Jens Mühle, Paul B. Krummel, Paul J. Fraser, and Hsiang-Jui Wang
Atmos. Meas. Tech., 14, 5955–5976, https://doi.org/10.5194/amt-14-5955-2021, https://doi.org/10.5194/amt-14-5955-2021, 2021
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This paper presents the first observations of atmospheric HFC-23 abundances with a ground-based remote sensing technique. The increasing trend of the HFC-23 abundances analyzed by this study agrees with that derived from other existing in situ measurements. This study indicates that ground-based FTIR observation has the capability to monitor the trend of atmospheric HFC-23 and could allow for monitoring the distribution of global atmospheric HFC-23 abundances in more detail.
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.
Fides Lefrancois, Markus Jesswein, Markus Thoma, Andreas Engel, Kieran Stanley, and Tanja Schuck
Atmos. Meas. Tech., 14, 4669–4687, https://doi.org/10.5194/amt-14-4669-2021, https://doi.org/10.5194/amt-14-4669-2021, 2021
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Synthetic halocarbons can contribute to stratospheric ozone depletion or to climate change. In many applications they have been replaced over the last years. The presented non-target analysis shows an application approach to quantify those replacements retrospectively, using recorded data of air measurements with gas chromatography coupled to time-of-flight mass spectrometry. We focus on the retrospective analysis of the fourth-generation halocarbons, detected at Taunus Observatory in Germany.
Felix Ploeger, Mohamadou Diallo, Edward Charlesworth, Paul Konopka, Bernard Legras, Johannes C. Laube, Jens-Uwe Grooß, Gebhard Günther, Andreas Engel, and Martin Riese
Atmos. Chem. Phys., 21, 8393–8412, https://doi.org/10.5194/acp-21-8393-2021, https://doi.org/10.5194/acp-21-8393-2021, 2021
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We investigate the global stratospheric circulation (Brewer–Dobson circulation) in the new ECMWF ERA5 reanalysis based on age of air simulations, and we compare it to results from the preceding ERA-Interim reanalysis. Our results show a slower stratospheric circulation and higher age for ERA5. The age of air trend in ERA5 over the 1989–2018 period is negative throughout the stratosphere, related to multi-annual variability and a potential contribution from changes in the reanalysis system.
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.
Thomas Wagenhäuser, Andreas Engel, and Robert Sitals
Atmos. Meas. Tech., 14, 3923–3934, https://doi.org/10.5194/amt-14-3923-2021, https://doi.org/10.5194/amt-14-3923-2021, 2021
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AirCore samplers are increasingly deployed to weather balloons to collect continuous atmospheric samples. We introduce a technique that can be used in situ to evaluate different data processing methods that are required to derive vertical trace gas profiles from AirCore measurements after sample recovery. Results from two test flights with a specific AirCore configuration provide evidence for systematic deviations in altitude attribution for the upper levels, which can be empirically corrected.
Daniel Say, Alistair J. Manning, Luke M. Western, Dickon Young, Adam Wisher, Matthew Rigby, Stefan Reimann, Martin K. Vollmer, Michela Maione, Jgor Arduini, Paul B. Krummel, Jens Mühle, Christina M. Harth, Brendan Evans, Ray F. Weiss, Ronald G. Prinn, and Simon O'Doherty
Atmos. Chem. Phys., 21, 2149–2164, https://doi.org/10.5194/acp-21-2149-2021, https://doi.org/10.5194/acp-21-2149-2021, 2021
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Perfluorocarbons (PFCs) are potent greenhouse gases with exceedingly long lifetimes. We used atmospheric measurements from a global monitoring network to track the accumulation of these gases in the atmosphere. In the case of the two most abundant PFCs, recent measurements indicate that global emissions are increasing. In Europe, we used a model to estimate regional PFC emissions. Our results show that there was no significant decline in northwest European PFC emissions between 2010 and 2019.
Rachel L. Tunnicliffe, Anita L. Ganesan, Robert J. Parker, Hartmut Boesch, Nicola Gedney, Benjamin Poulter, Zhen Zhang, Jošt V. Lavrič, David Walter, Matthew Rigby, Stephan Henne, Dickon Young, and Simon O'Doherty
Atmos. Chem. Phys., 20, 13041–13067, https://doi.org/10.5194/acp-20-13041-2020, https://doi.org/10.5194/acp-20-13041-2020, 2020
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This study quantifies Brazil’s emissions of a potent atmospheric greenhouse gas, methane. This is in the field of atmospheric modelling and uses remotely sensed data and surface measurements of methane concentrations as well as an atmospheric transport model to interpret the data. Because of Brazil’s large emissions from wetlands, agriculture and biomass burning, these emissions affect global methane concentrations and thus are of global significance.
Malte Meinshausen, Zebedee R. J. Nicholls, Jared Lewis, Matthew J. Gidden, Elisabeth Vogel, Mandy Freund, Urs Beyerle, Claudia Gessner, Alexander Nauels, Nico Bauer, Josep G. Canadell, John S. Daniel, Andrew John, Paul B. Krummel, Gunnar Luderer, Nicolai Meinshausen, Stephen A. Montzka, Peter J. Rayner, Stefan Reimann, Steven J. Smith, Marten van den Berg, Guus J. M. Velders, Martin K. Vollmer, and Ray H. J. Wang
Geosci. Model Dev., 13, 3571–3605, https://doi.org/10.5194/gmd-13-3571-2020, https://doi.org/10.5194/gmd-13-3571-2020, 2020
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This study provides the future greenhouse gas (GHG) concentrations under the new set of so-called SSP scenarios (the successors of the IPCC SRES and previous representative concentration pathway (RCP) scenarios). The projected CO2 concentrations range from 350 ppm for low-emission scenarios by 2150 to more than 2000 ppm under the high-emission scenarios. We also provide concentrations, latitudinal gradients, and seasonality for most of the other 42 considered GHGs.
Marius Hauck, Harald Bönisch, Peter Hoor, Timo Keber, Felix Ploeger, Tanja J. Schuck, and Andreas Engel
Atmos. Chem. Phys., 20, 8763–8785, https://doi.org/10.5194/acp-20-8763-2020, https://doi.org/10.5194/acp-20-8763-2020, 2020
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This study features an extended inversion method that includes transport across the extratropical tropopause to derive age spectra in the lowermost stratosphere from in situ trace gas measurements. The refined method is validated in a model setup and applied to data gained with the HALO research aircraft. Results are congruent with the findings of previous studies so that the method provides a promising toolset for the analysis of stratospheric dynamics based on observations in the future.
Frauke Fritsch, Hella Garny, Andreas Engel, Harald Bönisch, and Roland Eichinger
Atmos. Chem. Phys., 20, 8709–8725, https://doi.org/10.5194/acp-20-8709-2020, https://doi.org/10.5194/acp-20-8709-2020, 2020
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We test two methods to derive age of air as a diagnostic of the Brewer–Dobson circulation from non-linear increasing trace gases such as SF6 using a chemistry-climate model and observations. Both the model and the observations show systematic variation of the age of air trend dependent on the chosen assumptions that are required when deriving age of air from measurements. This provides insight into the differences in age of air trends of observations and models.
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.
Danilo Custodio, Ralf Ebinghaus, T. Gerard Spain, and Johannes Bieser
Atmos. Chem. Phys., 20, 7929–7939, https://doi.org/10.5194/acp-20-7929-2020, https://doi.org/10.5194/acp-20-7929-2020, 2020
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Using a stereo algorithm, we reconstructed 99.9 % of the total atmospheric gas mercury and presented a new insight into atmospheric mercury source assessing, which can have great relevance for policy and regulations in light of the Minamata convention.
Moya L. Macdonald, Jemma L. Wadham, Dickon Young, Chris R. Lunder, Ove Hermansen, Guillaume Lamarche-Gagnon, and Simon O'Doherty
Atmos. Chem. Phys., 20, 7243–7258, https://doi.org/10.5194/acp-20-7243-2020, https://doi.org/10.5194/acp-20-7243-2020, 2020
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Climate change has caused glaciers in the Arctic to shrink, uncovering new soils. We used field measurements to study the exchange of a group of gases involved in ozone destruction, called halocarbons, between these new soils and the atmosphere. We found that mats of cyanobacteria, early colonisers of soils, are linked to a larger-than-expected exchange of halocarbons with the atmosphere. We also found that gases which are commonly thought to be marine in origin were released from these soils.
Peter G. Simmonds, Matthew Rigby, Alistair J. Manning, Sunyoung Park, Kieran M. Stanley, Archie McCulloch, Stephan Henne, Francesco Graziosi, Michela Maione, Jgor Arduini, Stefan Reimann, Martin K. Vollmer, Jens Mühle, Simon O'Doherty, Dickon Young, Paul B. Krummel, Paul J. Fraser, Ray F. Weiss, Peter K. Salameh, Christina M. Harth, Mi-Kyung Park, Hyeri Park, Tim Arnold, Chris Rennick, L. Paul Steele, Blagoj Mitrevski, Ray H. J. Wang, and Ronald G. Prinn
Atmos. Chem. Phys., 20, 7271–7290, https://doi.org/10.5194/acp-20-7271-2020, https://doi.org/10.5194/acp-20-7271-2020, 2020
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Sulfur hexafluoride (SF6) is a potent greenhouse gas which is regulated under the Kyoto Protocol. From a 40-year record of measurements, collected at five global monitoring sites and archived air samples, we show that its concentration in the atmosphere has steadily increased. Using modelling techniques, we estimate that global emissions have increased by about 24 % over the past decade. We find that this increase is driven by the demand for SF6-insulated switchgear in developing countries.
Luke M. Western, Zhe Sha, Matthew Rigby, Anita L. Ganesan, Alistair J. Manning, Kieran M. Stanley, Simon J. O'Doherty, Dickon Young, and Jonathan Rougier
Geosci. Model Dev., 13, 2095–2107, https://doi.org/10.5194/gmd-13-2095-2020, https://doi.org/10.5194/gmd-13-2095-2020, 2020
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Assessments of greenhouse gas emissions using atmospheric measurements and meteorological models, or
top-downmethods, are important to verify national inventories or produce a stand-alone estimate where no inventory exists. We present a novel top-down method to estimate emissions. This approach uses a fast method called an integrated nested Laplacian approximation to estimate how these emissions are correlated with other emissions in different locations and at different times.
Elise S. Droste, Karina E. Adcock, Matthew J. Ashfold, Charles Chou, Zoë Fleming, Paul J. Fraser, Lauren J. Gooch, Andrew J. Hind, Ray L. Langenfelds, Emma C. Leedham Elvidge, Norfazrin Mohd Hanif, Simon O'Doherty, David E. Oram, Chang-Feng Ou-Yang, Marios Panagi, Claire E. Reeves, William T. Sturges, and Johannes C. Laube
Atmos. Chem. Phys., 20, 4787–4807, https://doi.org/10.5194/acp-20-4787-2020, https://doi.org/10.5194/acp-20-4787-2020, 2020
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We update the tropospheric trends and emissions of six perfluorocarbon (PFC) gases, including separate isomers. Trends for these strong greenhouse gases are still increasing, but at slower rates than previously. The lack of natural sinks results in the global accumulation of 833 million metric tonnes of CO2 equivalent for these six PFCs by 2017. Modelling results indicate potential source regions and types in East Asia, but we find that many emissions are unaccounted for in emission reports.
Timo Keber, Harald Bönisch, Carl Hartick, Marius Hauck, Fides Lefrancois, Florian Obersteiner, Akima Ringsdorf, Nils Schohl, Tanja Schuck, Ryan Hossaini, Phoebe Graf, Patrick Jöckel, and Andreas Engel
Atmos. Chem. Phys., 20, 4105–4132, https://doi.org/10.5194/acp-20-4105-2020, https://doi.org/10.5194/acp-20-4105-2020, 2020
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In this paper we summarize observations of short-lived halocarbons in the tropopause region. We show that, especially during winter, the levels of short-lived bromine gases at the extratropical tropopause are higher than at the tropical tropopause. We discuss the impact of the distributions on stratospheric bromine levels and compare our observations to two models with four different emission scenarios.
Anna Karion, William Callahan, Michael Stock, Steve Prinzivalli, Kristal R. Verhulst, Jooil Kim, Peter K. Salameh, Israel Lopez-Coto, and James Whetstone
Earth Syst. Sci. Data, 12, 699–717, https://doi.org/10.5194/essd-12-699-2020, https://doi.org/10.5194/essd-12-699-2020, 2020
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Our paper presents atmospheric concentrations of carbon dioxide and methane in the northeastern United States. We also describe the collection, quality control, and uncertainty estimation methods associated with the observations. The network is composed of 23 tower-based stations, including a dense sub-network in the Washington, DC, and Baltimore, Maryland, urban areas. Observations can be used to assess greenhouse gas emissions from these cities and regions.
Tanja J. Schuck, Ann-Katrin Blank, Elisa Rittmeier, Jonathan Williams, Carl A. M. Brenninkmeijer, Andreas Engel, and Andreas Zahn
Atmos. Meas. Tech., 13, 73–84, https://doi.org/10.5194/amt-13-73-2020, https://doi.org/10.5194/amt-13-73-2020, 2020
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Air sample collection aboard aircraft is a tool to measure atmospheric trace gas mixing ratios at altitude. We present results on the stability of 28 halocarbons during storage of air samples collected in stainless-steel flasks inside an automated air sampling unit which is part of the CARIBIC instrument package. Selected fluorinated compounds grew during the experiments while short-lived compounds were depleted. Individual substances were additionally influenced by high mixing ratios of ozone.
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.
Maxime Prignon, Simon Chabrillat, Daniele Minganti, Simon O'Doherty, Christian Servais, Gabriele Stiller, Geoffrey C. Toon, Martin K. Vollmer, and Emmanuel Mahieu
Atmos. Chem. Phys., 19, 12309–12324, https://doi.org/10.5194/acp-19-12309-2019, https://doi.org/10.5194/acp-19-12309-2019, 2019
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Hydrochlorofluorocarbons (HCFCs) are the first, but temporary, substitution products for the strong ozone-depleting chlorofluorocarbons (CFCs). In this work, we present and validate an improved method to retrieve the most abundant HCFC in the atmosphere, allowing its evolution to be monitored independently in the troposphere and stratosphere. These kinds of contributions are fundamental for scrutinizing the fulfilment of the Montreal Protocol on Substances that Deplete the Ozone Layer.
Andreas Marsing, Tina Jurkat-Witschas, Jens-Uwe Grooß, Stefan Kaufmann, Romy Heller, Andreas Engel, Peter Hoor, Jens Krause, and Christiane Voigt
Atmos. Chem. Phys., 19, 10757–10772, https://doi.org/10.5194/acp-19-10757-2019, https://doi.org/10.5194/acp-19-10757-2019, 2019
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We study the partitioning of inorganic chlorine into active (ozone-depleting) and reservoir species in the lowermost stratosphere of the Arctic polar vortex, using novel in situ aircraft measurements in winter 2015/2016. We observe a change in recovery pathways of the reservoirs HCl and ClONO2 with increasing potential temperature. A comparison with the CLaMS model relates the observations to the vortex-wide evolution and confirms unresolved discrepancies in the mid-winter HCl distribution.
Ann R. Stavert, Simon O'Doherty, Kieran Stanley, Dickon Young, Alistair J. Manning, Mark F. Lunt, Christopher Rennick, and Tim Arnold
Atmos. Meas. Tech., 12, 4495–4518, https://doi.org/10.5194/amt-12-4495-2019, https://doi.org/10.5194/amt-12-4495-2019, 2019
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Under the UK GAUGE project, two new greenhouse gas observation sites were established in the 2013/2014 winter at two telecommunications towers. A combination of spectroscopic and chromatographic instrumentation was used to measure CO2, CH4, CO, N2O and SF6. The advantages and disadvantages of two CRDS sample drying strategies, Nafion(R) and empirical water correction, were also examined.
Jens Mühle, Cathy M. Trudinger, Luke M. Western, Matthew Rigby, Martin K. Vollmer, Sunyoung Park, Alistair J. Manning, Daniel Say, Anita Ganesan, L. Paul Steele, Diane J. Ivy, Tim Arnold, Shanlan Li, Andreas Stohl, Christina M. Harth, Peter K. Salameh, Archie McCulloch, Simon O'Doherty, Mi-Kyung Park, Chun Ok Jo, Dickon Young, Kieran M. Stanley, Paul B. Krummel, Blagoj Mitrevski, Ove Hermansen, Chris Lunder, Nikolaos Evangeliou, Bo Yao, Jooil Kim, Benjamin Hmiel, Christo Buizert, Vasilii V. Petrenko, Jgor Arduini, Michela Maione, David M. Etheridge, Eleni Michalopoulou, Mike Czerniak, Jeffrey P. Severinghaus, Stefan Reimann, Peter G. Simmonds, Paul J. Fraser, Ronald G. Prinn, and Ray F. Weiss
Atmos. Chem. Phys., 19, 10335–10359, https://doi.org/10.5194/acp-19-10335-2019, https://doi.org/10.5194/acp-19-10335-2019, 2019
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We discuss atmospheric concentrations and emissions of the strong greenhouse gas perfluorocyclobutane. A large fraction of recent emissions stem from China, India, and Russia, probably as a by-product from the production of fluoropolymers and fluorochemicals. Most historic emissions likely stem from developed countries. Total emissions are higher than what is being reported. Clearly, more measurements and better reporting are needed to understand emissions of this and other greenhouse gases.
Daniel Say, Anita L. Ganesan, Mark F. Lunt, Matthew Rigby, Simon O'Doherty, Christina Harth, Alistair J. Manning, Paul B. Krummel, and Stephane Bauguitte
Atmos. Chem. Phys., 19, 9865–9885, https://doi.org/10.5194/acp-19-9865-2019, https://doi.org/10.5194/acp-19-9865-2019, 2019
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Despite its emergence as a global economic power, very little information exists regarding India's halocarbon (CFC, HCFC, HFC and chlorocarbon) emissions. We report atmospheric measurements of these gases from above India, and use them to estimate India's emissions. Our results are consistent with the emissions profile of a developing country, with large emissions of HCFCs, HFCs and chlorocarbons not regulated under the Montreal Protocol, but little evidence for ongoing CFC consumption.
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.
Joseph R. Pitt, Grant Allen, Stéphane J.-B. Bauguitte, Martin W. Gallagher, James D. Lee, Will Drysdale, Beth Nelson, Alistair J. Manning, and Paul I. Palmer
Atmos. Chem. Phys., 19, 8931–8945, https://doi.org/10.5194/acp-19-8931-2019, https://doi.org/10.5194/acp-19-8931-2019, 2019
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This paper presents a new method to assess inventory estimates of greenhouse gas and air pollutant emissions for large cities and their surrounding regions. A case study using data sampled by a research aircraft around London was used to test the method. We found that the UK national inventory agrees with our observations for CO but needed lower emissions for CH4 to agree with the measured data. Repeated studies could help determine how these emissions vary on different timescales.
David D. Parrish, Richard G. Derwent, Simon O'Doherty, and Peter G. Simmonds
Atmos. Meas. Tech., 12, 3383–3394, https://doi.org/10.5194/amt-12-3383-2019, https://doi.org/10.5194/amt-12-3383-2019, 2019
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We present a flexible method that employs a power series expansion and Fourier series analysis to characterize the average long-term change and seasonal cycle, respectively, from a time series of observations of a trace atmospheric species. This approach maximizes the statistically significant information derived, including non-linear aspects of the long-term trends, without over fitting the data. Generally, a small set of parameter values (e.g., 7 or 8) provides this characterization.
Ruhi S. Humphries, Ian M. McRobert, Will A. Ponsonby, Jason P. Ward, Melita D. Keywood, Zoe M. Loh, Paul B. Krummel, and James Harnwell
Atmos. Meas. Tech., 12, 3019–3038, https://doi.org/10.5194/amt-12-3019-2019, https://doi.org/10.5194/amt-12-3019-2019, 2019
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Undertaking atmospheric observations from ships provides important data in regions where measurements are impossible by other means. However, making measurements so close to a diesel exhaust plume is difficult. In this paper, we describe an algorithm that utilises ongoing measurements of aerosol number concentrations, black carbon mass concentrations, and mixing ratios of carbon monoxide and carbon dioxide to accurately distinguish between exhaust and background data periods.
Felix Ploeger, Bernard Legras, Edward Charlesworth, Xiaolu Yan, Mohamadou Diallo, Paul Konopka, Thomas Birner, Mengchu Tao, Andreas Engel, and Martin Riese
Atmos. Chem. Phys., 19, 6085–6105, https://doi.org/10.5194/acp-19-6085-2019, https://doi.org/10.5194/acp-19-6085-2019, 2019
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We analyse the change in the circulation of the middle atmosphere based on current generation meteorological reanalysis data sets. We find that long-term changes from 1989 to 2015 are similar for the chosen reanalyses, mainly resembling the forced response in climate model simulations to climate change. For shorter periods circulation changes are less robust, and the representation of decadal variability appears to be a major uncertainty for modelling the circulation of the middle atmosphere.
Marius Hauck, Frauke Fritsch, Hella Garny, and Andreas Engel
Atmos. Chem. Phys., 19, 5269–5291, https://doi.org/10.5194/acp-19-5269-2019, https://doi.org/10.5194/acp-19-5269-2019, 2019
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The paper presents a modified method to invert mixing ratios of chemically active tracers into stratospheric age spectra. It features an imposed seasonal cycle to include transport seasonality into the spectra. An idealized set of tracers from a model is used as proof of concept and results are in good agreement with the model reference, except for the lowermost stratosphere. Applicability is studied with focus on number of tracers and error tolerance, providing a starting point for future work.
Emily D. White, Matthew Rigby, Mark F. Lunt, T. Luke Smallman, Edward Comyn-Platt, Alistair J. Manning, Anita L. Ganesan, Simon O'Doherty, Ann R. Stavert, Kieran Stanley, Mathew Williams, Peter Levy, Michel Ramonet, Grant L. Forster, Andrew C. Manning, and Paul I. Palmer
Atmos. Chem. Phys., 19, 4345–4365, https://doi.org/10.5194/acp-19-4345-2019, https://doi.org/10.5194/acp-19-4345-2019, 2019
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Understanding carbon dioxide (CO2) fluxes from the terrestrial biosphere on a national scale is important for evaluating land use strategies to mitigate climate change. We estimate emissions of CO2 from the UK biosphere using atmospheric data in a top-down approach. Our findings show that bottom-up estimates from models of biospheric fluxes overestimate the amount of CO2 uptake in summer. This suggests these models wrongly estimate or omit key processes, e.g. land disturbance due to harvest.
Martin K. Vollmer, François Bernard, Blagoj Mitrevski, L. Paul Steele, Cathy M. Trudinger, Stefan Reimann, Ray L. Langenfelds, Paul B. Krummel, Paul J. Fraser, David M. Etheridge, Mark A. J. Curran, and James B. Burkholder
Atmos. Chem. Phys., 19, 3481–3492, https://doi.org/10.5194/acp-19-3481-2019, https://doi.org/10.5194/acp-19-3481-2019, 2019
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We have discovered a new compound in the atmosphere, octafluorooxolane (c-C4F8O), from measurements in archived air samples. From our laboratory studies, we find that c-C4F8O is a very powerful greenhouse gas thereby contributing to global warming, and that it has a very long atmospheric lifetime of more than 3500 years. Based on our measurements we could reconstruct its atmospheric evolution over more than 4 decades. Based on this, we could estimate the global emissions of c-C4F8O.
Carole Helfter, Neil Mullinger, Massimo Vieno, Simon O'Doherty, Michel Ramonet, Paul I. Palmer, and Eiko Nemitz
Atmos. Chem. Phys., 19, 3043–3063, https://doi.org/10.5194/acp-19-3043-2019, https://doi.org/10.5194/acp-19-3043-2019, 2019
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We present a novel approach to estimate the annual budgets of carbon dioxide (881.0 ± 128.5 Tg) and methane (2.55 ± 0.48 Tg) of the British Isles from shipborne measurements taken over a 3-year period (2015–2017). This study brings independent verification of the emission budgets estimated using alternative products and investigates the seasonality of these emissions, which is usually not possible.
Kieran Brophy, Heather Graven, Alistair J. Manning, Emily White, Tim Arnold, Marc L. Fischer, Seongeun Jeong, Xinguang Cui, and Matthew Rigby
Atmos. Chem. Phys., 19, 2991–3006, https://doi.org/10.5194/acp-19-2991-2019, https://doi.org/10.5194/acp-19-2991-2019, 2019
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We investigate potential errors and uncertainties related to the spatial and temporal prior representation of emissions and modelled atmospheric transport for the inversion of California's fossil fuel CO2 emissions. Our results indicate that uncertainties in posterior total state fossil fuel CO2 estimates arising from the choice of prior emissions or atmospheric transport model are on the order of 15 % or less for the ground-based network in California we consider.
Daniel Say, Anita L. Ganesan, Mark F. Lunt, Matthew Rigby, Simon O'Doherty, Chris Harth, Alistair J. Manning, Paul B. Krummel, and Stephane Bauguitte
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-1287, https://doi.org/10.5194/acp-2018-1287, 2019
Publication in ACP not foreseen
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India is a potentially significant source of chlorocarbons, gases typically used as solvents and feedstocks. Given the potential for these species to deplete stratospheric ozone, understanding their sources is important. We use flask measurements collected from an aircraft to infer India's chlorocarbon emissions. We link emissions of carbon tetrachloride to the industrial production of other chloromethanes, and provide evidence for rapid growth in India's emissions of dichloromethane.
Ann R. Stavert, Rachel M. Law, Marcel van der Schoot, Ray L. Langenfelds, Darren A. Spencer, Paul B. Krummel, Scott D. Chambers, Alistair G. Williams, Sylvester Werczynski, Roger J. Francey, and Russell T. Howden
Atmos. Meas. Tech., 12, 1103–1121, https://doi.org/10.5194/amt-12-1103-2019, https://doi.org/10.5194/amt-12-1103-2019, 2019
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The Southern Ocean is a key sink of carbon dioxide (CO2), but efforts to study trends in and the variability of the sink have been hindered by the limited number of CO2 measurements in this region. Here we describe a set of new in situ continuous (minutely) atmospheric CO2 observations. We show that this new record better captures long-term changes and seasonality than traditional 2-weekly flask records. As such, this data set will provide key insights into the changing Southern Ocean sink.
Pingyang Li, Jens Mühle, Stephen A. Montzka, David E. Oram, Benjamin R. Miller, Ray F. Weiss, Paul J. Fraser, and Toste Tanhua
Ocean Sci., 15, 33–60, https://doi.org/10.5194/os-15-33-2019, https://doi.org/10.5194/os-15-33-2019, 2019
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Use of CFCs as oceanic transient tracers is difficult for recently ventilated water masses as their atmospheric mole fractions have been decreasing. To explore novel tracers, we synthesized consistent annual mean atmospheric histories of HCFC-22, HCFC-141b, HCFC-142b, HFC-134a, HFC-125, HFC-23, PFC-14 (CF4) and PFC-116 in both hemispheres and reconstructed their solubility functions in water and seawater. This work is also potentially useful for tracer studies in a range of natural waters.
Sarah Connors, Alistair J. Manning, Andrew D. Robinson, Stuart N. Riddick, Grant L. Forster, Anita Ganesan, Aoife Grant, Stephen Humphrey, Simon O'Doherty, Dave E. Oram, Paul I. Palmer, Robert L. Skelton, Kieran Stanley, Ann Stavert, Dickon Young, and Neil R. P. Harris
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-1187, https://doi.org/10.5194/acp-2018-1187, 2018
Preprint withdrawn
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Methane is an important greenhouse gas & reducing its emissions is a vital part of climate change mitigation to limit global temperature increase to 1.5 °C or 2.0 °C. This paper explains a way to estimate emitted methane over a sub-national area by combining measurements & computer dispersion modelling in a so-called
inversiontechnique. Compared with the current national inventory, our results show lower emissions for Cambridgeshire, possibly due to waste sector emission differences.
Tanja J. Schuck, Fides Lefrancois, Franziska Gallmann, Danrong Wang, Markus Jesswein, Jesica Hoker, Harald Bönisch, and Andreas Engel
Atmos. Chem. Phys., 18, 16553–16569, https://doi.org/10.5194/acp-18-16553-2018, https://doi.org/10.5194/acp-18-16553-2018, 2018
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We present the first results of regular halocarbon measurements at Taunus Observatory, Germany. Halogenated gases contribute to stratospheric ozone depletion and to radiative forcing. Time-of-flight mass spectrometry allows one to assess a large number of compounds; the measurements are expected to provide better constraints for European emission estimates. CFC-11 and CFC-12 show small unexpected differences regarding outlier occurrence and seasonality, indicating ongoing emissions of CFC-11.
Simon Chabrillat, Corinne Vigouroux, Yves Christophe, Andreas Engel, Quentin Errera, Daniele Minganti, Beatriz M. Monge-Sanz, Arjo Segers, and Emmanuel Mahieu
Atmos. Chem. Phys., 18, 14715–14735, https://doi.org/10.5194/acp-18-14715-2018, https://doi.org/10.5194/acp-18-14715-2018, 2018
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Mean age of stratospheric air is computed for the period 1989–2015 with a kinematic transport model which uses surface pressure and wind fields from five reanalyses: ERA-I, MERRA-2, MERRA, CFSR, JRA-55. The spread between the resulting datasets is as large as in climate model intercomparisons; the age trends have large disagreement and depend strongly on the considered period. We highlight the need for similar studies using diabatic transport models which also use temperature and heating rates.
Tim Arnold, Alistair J. Manning, Jooil Kim, Shanlan Li, Helen Webster, David Thomson, Jens Mühle, Ray F. Weiss, Sunyoung Park, and Simon O'Doherty
Atmos. Chem. Phys., 18, 13305–13320, https://doi.org/10.5194/acp-18-13305-2018, https://doi.org/10.5194/acp-18-13305-2018, 2018
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Emissions of carbon tetrafluoride CF4, NF3 and CHF3 in east Asia have been calculated using atmospheric measurements and an atmospheric transport model. We calculate emissions of CF4 to be quite constant between the years 2008 and 2015 for both China and South Korea, with 2015 emissions calculated at 4.33 ± 2.65 Gg yr-1 and 0.36 ± 0.11 Gg yr-1, respectively. Emission estimates of NF3 from South Korea could be made with relatively small uncertainty at 0.6 ± 0.07 Gg yr-1 in 2015.
Paul I. Palmer, Simon O'Doherty, Grant Allen, Keith Bower, Hartmut Bösch, Martyn P. Chipperfield, Sarah Connors, Sandip Dhomse, Liang Feng, Douglas P. Finch, Martin W. Gallagher, Emanuel Gloor, Siegfried Gonzi, Neil R. P. Harris, Carole Helfter, Neil Humpage, Brian Kerridge, Diane Knappett, Roderic L. Jones, Michael Le Breton, Mark F. Lunt, Alistair J. Manning, Stephan Matthiesen, Jennifer B. A. Muller, Neil Mullinger, Eiko Nemitz, Sebastian O'Shea, Robert J. Parker, Carl J. Percival, Joseph Pitt, Stuart N. Riddick, Matthew Rigby, Harjinder Sembhi, Richard Siddans, Robert L. Skelton, Paul Smith, Hannah Sonderfeld, Kieran Stanley, Ann R. Stavert, Angelina Wenger, Emily White, Christopher Wilson, and Dickon Young
Atmos. Chem. Phys., 18, 11753–11777, https://doi.org/10.5194/acp-18-11753-2018, https://doi.org/10.5194/acp-18-11753-2018, 2018
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This paper provides an overview of the Greenhouse gAs Uk and Global Emissions (GAUGE) experiment. GAUGE was designed to quantify nationwide GHG emissions of the UK, bringing together measurements and atmospheric transport models. This novel experiment is the first of its kind. We anticipate it will inform the blueprint for countries that are building a measurement infrastructure in preparation for global stocktakes, which are a key part of the Paris Agreement.
Sunyoung Park, Shanlan Li, Jens Mühle, Simon O'Doherty, Ray F. Weiss, Xuekun Fang, Stefan Reimann, and Ronald G. Prinn
Atmos. Chem. Phys., 18, 11729–11738, https://doi.org/10.5194/acp-18-11729-2018, https://doi.org/10.5194/acp-18-11729-2018, 2018
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Multi-year, real-time atmospheric carbon tetrachloride (CCl4) record obtained at Gosan station (33° N, 126° E) presents evidence of significant unreported emissions of this first-generation ozone-depleting substance. The missing emissions (~ 19 Gg yr−1) for China contribute to approximately 54 % of global emissions and are most likely related to CCl4 escape occurring during the production of chlorinated compounds and their usage as feedstocks and process agents in chemical manufacturing industries.
Sören Johansson, Wolfgang Woiwode, Michael Höpfner, Felix Friedl-Vallon, Anne Kleinert, Erik Kretschmer, Thomas Latzko, Johannes Orphal, Peter Preusse, Jörn Ungermann, Michelle L. Santee, Tina Jurkat-Witschas, Andreas Marsing, Christiane Voigt, Andreas Giez, Martina Krämer, Christian Rolf, Andreas Zahn, Andreas Engel, Björn-Martin Sinnhuber, and Hermann Oelhaf
Atmos. Meas. Tech., 11, 4737–4756, https://doi.org/10.5194/amt-11-4737-2018, https://doi.org/10.5194/amt-11-4737-2018, 2018
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We present two-dimensional cross sections of temperature, HNO3, O3, ClONO2, H2O and CFC-12 from measurements of the GLORIA infrared limb imager during the POLSTRACC/GW-LCYCLE/SALSA aircraft campaigns in the Arctic winter 2015/2016. GLORIA sounded the atmosphere between 5 and 14 km with vertical resolutions of 0.4–1 km. Estimated errors are in the range of 1–2 K (temperature) and 10 %–20 % (trace gases). Comparisons to in situ instruments onboard the aircraft and to Aura/MLS are shown.
Myriam Guillevic, Martin K. Vollmer, Simon A. Wyss, Daiana Leuenberger, Andreas Ackermann, Céline Pascale, Bernhard Niederhauser, and Stefan Reimann
Atmos. Meas. Tech., 11, 3351–3372, https://doi.org/10.5194/amt-11-3351-2018, https://doi.org/10.5194/amt-11-3351-2018, 2018
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We present new primary calibration scales for five halogenated greenhouse gases. The preparation method, newly applied to halocarbons, is dynamic and gravimetric
and allows the generation of reference gas mixtures at near-ambient levels (pmol mol−1). Each prepared molar fraction is traceable to the
realisation of SI units (International System of Units) and is assigned an uncertainty estimate following international guidelines.
Ronald G. Prinn, Ray F. Weiss, Jgor Arduini, Tim Arnold, H. Langley DeWitt, Paul J. Fraser, Anita L. Ganesan, Jimmy Gasore, Christina M. Harth, Ove Hermansen, Jooil Kim, Paul B. Krummel, Shanlan Li, Zoë M. Loh, Chris R. Lunder, Michela Maione, Alistair J. Manning, Ben R. Miller, Blagoj Mitrevski, Jens Mühle, Simon O'Doherty, Sunyoung Park, Stefan Reimann, Matt Rigby, Takuya Saito, Peter K. Salameh, Roland Schmidt, Peter G. Simmonds, L. Paul Steele, Martin K. Vollmer, Ray H. Wang, Bo Yao, Yoko Yokouchi, Dickon Young, and Lingxi Zhou
Earth Syst. Sci. Data, 10, 985–1018, https://doi.org/10.5194/essd-10-985-2018, https://doi.org/10.5194/essd-10-985-2018, 2018
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We present the data and accomplishments of the multinational global atmospheric measurement program AGAGE (Advanced Global Atmospheric Gases Experiment). At high frequency and at multiple sites, AGAGE measures all the important chemicals in the Montreal Protocol for the protection of the ozone layer and the non-carbon-dioxide gases assessed by the Intergovernmental Panel on Climate Change. AGAGE uses these data to estimate sources and sinks of all these gases and has operated since 1978.
Jens Krause, Peter Hoor, Andreas Engel, Felix Plöger, Jens-Uwe Grooß, Harald Bönisch, Timo Keber, Björn-Martin Sinnhuber, Wolfgang Woiwode, and Hermann Oelhaf
Atmos. Chem. Phys., 18, 6057–6073, https://doi.org/10.5194/acp-18-6057-2018, https://doi.org/10.5194/acp-18-6057-2018, 2018
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We present tracer measurements of CO and N2O measured during the POLSTRACC aircraft campaign in winter 2015–2016. We found enhanced CO values relative to N2O in the polar lower stratosphere in addition to the ageing of this region during winter. By using model simulations it was possible to link this enhancement to an increased mixing of the tropical tropopause. We thus conclude that the polar lower stratosphere in late winter is strongly influenced by quasi-isentropic mixing from the tropics.
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
Peter G. Simmonds, Matthew Rigby, Archie McCulloch, Martin K. Vollmer, Stephan Henne, Jens Mühle, Simon O'Doherty, Alistair J. Manning, Paul B. Krummel, Paul J. Fraser, Dickon Young, Ray F. Weiss, Peter K. Salameh, Christina M. Harth, Stefan Reimann, Cathy M. Trudinger, L. Paul Steele, Ray H. J. Wang, Diane J. Ivy, Ronald G. Prinn, Blagoj Mitrevski, and David M. Etheridge
Atmos. Chem. Phys., 18, 4153–4169, https://doi.org/10.5194/acp-18-4153-2018, https://doi.org/10.5194/acp-18-4153-2018, 2018
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Recent measurements of the potent greenhouse gas HFC-23, a by-product of HCFC-22 production, show a 28 % increase in the atmospheric mole fraction from 2009 to 2016. A minimum in the atmospheric abundance of HFC-23 in 2009 was attributed to abatement of HFC-23 emissions by incineration under the Clean Development Mechanism (CDM). Our results indicate that the recent increase in HFC-23 emissions is driven by failure of mitigation under the CDM to keep pace with increased HCFC-22 production.
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 %.
Isabelle Pison, Antoine Berchet, Marielle Saunois, Philippe Bousquet, Grégoire Broquet, Sébastien Conil, Marc Delmotte, Anita Ganesan, Olivier Laurent, Damien Martin, Simon O'Doherty, Michel Ramonet, T. Gerard Spain, Alex Vermeulen, and Camille Yver Kwok
Atmos. Chem. Phys., 18, 3779–3798, https://doi.org/10.5194/acp-18-3779-2018, https://doi.org/10.5194/acp-18-3779-2018, 2018
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Methane emissions on the national scale in France in 2012 are inferred by assimilating continuous atmospheric mixing ratio measurements from nine stations of the European network ICOS. Two complementary inversion set-ups are computed and analysed: (i) a regional run correcting for the spatial distribution of fluxes in France and (ii) a sectorial run correcting fluxes for activity sectors on the national scale. The results are compared with existing inventories and other regional inversions.
Kieran M. Stanley, Aoife Grant, Simon O'Doherty, Dickon Young, Alistair J. Manning, Ann R. Stavert, T. Gerard Spain, Peter K. Salameh, Christina M. Harth, Peter G. Simmonds, William T. Sturges, David E. Oram, and Richard G. Derwent
Atmos. Meas. Tech., 11, 1437–1458, https://doi.org/10.5194/amt-11-1437-2018, https://doi.org/10.5194/amt-11-1437-2018, 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.
Irène Xueref-Remy, Elsa Dieudonné, Cyrille Vuillemin, Morgan Lopez, Christine Lac, Martina Schmidt, Marc Delmotte, Frédéric Chevallier, François Ravetta, Olivier Perrussel, Philippe Ciais, François-Marie Bréon, Grégoire Broquet, Michel Ramonet, T. Gerard Spain, and Christophe Ampe
Atmos. Chem. Phys., 18, 3335–3362, https://doi.org/10.5194/acp-18-3335-2018, https://doi.org/10.5194/acp-18-3335-2018, 2018
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Urbanized and industrialized areas are the largest source of fossil CO2. This work analyses the atmospheric CO2 variability observed from the first in situ network deployed in the Paris megacity area. Gradients of several ppm are found between the rural, peri-urban and urban sites at the diurnal to the seasonal scales. Wind direction and speed as well as boundary layer dynamics, correlated to highly variable urban emissions, are shown to be key regulator factors of the observed CO2 records.
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.
Martin K. Vollmer, Dickon Young, Cathy M. Trudinger, Jens Mühle, Stephan Henne, Matthew Rigby, Sunyoung Park, Shanlan Li, Myriam Guillevic, Blagoj Mitrevski, Christina M. Harth, Benjamin R. Miller, Stefan Reimann, Bo Yao, L. Paul Steele, Simon A. Wyss, Chris R. Lunder, Jgor Arduini, Archie McCulloch, Songhao Wu, Tae Siek Rhee, Ray H. J. Wang, Peter K. Salameh, Ove Hermansen, Matthias Hill, Ray L. Langenfelds, Diane Ivy, Simon O'Doherty, Paul B. Krummel, Michela Maione, David M. Etheridge, Lingxi Zhou, Paul J. Fraser, Ronald G. Prinn, Ray F. Weiss, and Peter G. Simmonds
Atmos. Chem. Phys., 18, 979–1002, https://doi.org/10.5194/acp-18-979-2018, https://doi.org/10.5194/acp-18-979-2018, 2018
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We measured the three chlorofluorocarbons (CFCs) CFC-13, CFC-114, and CFC-115 in the atmosphere because they are important in stratospheric ozone depletion. These compounds should have decreased in the atmosphere because they are banned by the Montreal Protocol but we find the opposite. Emissions over the last decade have not declined on a global scale. We use inverse modeling and our observations to find that a large part of the emissions originate in the Asian region.
Kelley C. Wells, Dylan B. Millet, Nicolas Bousserez, Daven K. Henze, Timothy J. Griffis, Sreelekha Chaliyakunnel, Edward J. Dlugokencky, Eri Saikawa, Gao Xiang, Ronald G. Prinn, Simon O'Doherty, Dickon Young, Ray F. Weiss, Geoff S. Dutton, James W. Elkins, Paul B. Krummel, Ray Langenfelds, and L. Paul Steele
Atmos. Chem. Phys., 18, 735–756, https://doi.org/10.5194/acp-18-735-2018, https://doi.org/10.5194/acp-18-735-2018, 2018
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This paper uses three different frameworks to derive nitrous oxide (N2O) emissions based on global surface observations. One of these frameworks employs a new approach that allows for fast computation and explores a larger solution space than other methods. Our results point to a few conclusions about the global N2O budget, including a larger contribution from tropical sources, an overestimate of natural soil emissions, and an underestimate of agricultural sources particularly in springtime.
Andreas Engel, Harald Bönisch, Jennifer Ostermöller, Martyn P. Chipperfield, Sandip Dhomse, and Patrick Jöckel
Atmos. Chem. Phys., 18, 601–619, https://doi.org/10.5194/acp-18-601-2018, https://doi.org/10.5194/acp-18-601-2018, 2018
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We present a new method to derive equivalent effective stratospheric chlorine (EESC), which is based on an improved formulation of the propagation of trends of species with chemical loss from the troposphere to the stratosphere. EESC calculated with the new method shows much better agreement with model-derived ESC. Based on this new formulation, we expect the halogen impact on midlatitude stratospheric ozone to return to 1980 values about 10 years later, then using the current formulation.
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.
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.
Ellen Eckert, Thomas von Clarmann, Alexandra Laeng, Gabriele P. Stiller, Bernd Funke, Norbert Glatthor, Udo Grabowski, Sylvia Kellmann, Michael Kiefer, Andrea Linden, Arne Babenhauserheide, Gerald Wetzel, Christopher Boone, Andreas Engel, Jeremy J. Harrison, Patrick E. Sheese, Kaley A. Walker, and Peter F. Bernath
Atmos. Meas. Tech., 10, 2727–2743, https://doi.org/10.5194/amt-10-2727-2017, https://doi.org/10.5194/amt-10-2727-2017, 2017
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We retrieved vertical profiles of CCl4 from MIPAS Envisat IMK/IAA data. A detailed description of all characteristics is included in the paper as well as comparisons with historical measurements and comparisons with collocated measurements of instruments covering the same time span as MIPAS Envisat. A particular focus also lies on the usage of a new CCl4 spectroscopic dataset introduced recently, which leads to more realistic CCl4 volume mixing ratios.
Kristal R. Verhulst, Anna Karion, Jooil Kim, Peter K. Salameh, Ralph F. Keeling, Sally Newman, John Miller, Christopher Sloop, Thomas Pongetti, Preeti Rao, Clare Wong, Francesca M. Hopkins, Vineet Yadav, Ray F. Weiss, Riley M. Duren, and Charles E. Miller
Atmos. Chem. Phys., 17, 8313–8341, https://doi.org/10.5194/acp-17-8313-2017, https://doi.org/10.5194/acp-17-8313-2017, 2017
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We present the first carbon dioxide (CO2) and methane (CH4) measurements from an extensive surface network as part of the Los Angeles Megacity Carbon Project. We describe methods that are essential for understanding carbon fluxes from complex urban environments. CO2 and CH4 levels are spatially and temporally variable, with urban sites showing significant enhancements relative to background. In 2015, the median afternoon enhancement near downtown Los Angeles was ~15 ppm CO2 and ~80 ppb CH4.
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.
Olivier Membrive, Cyril Crevoisier, Colm Sweeney, François Danis, Albert Hertzog, Andreas Engel, Harald Bönisch, and Laurence Picon
Atmos. Meas. Tech., 10, 2163–2181, https://doi.org/10.5194/amt-10-2163-2017, https://doi.org/10.5194/amt-10-2163-2017, 2017
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A new high-resolution AirCore system is presented. This system flown with stratospheric balloons allows us to sample atmospheric air during the descent. The analysis of trace gases (CO2 and CH4 in this case) in the collected air sample provides information on the vertical distribution along the atmospheric column. The continuous vertical profiles retrieved may contribute to several research topics concerning the observation of greenhouse gases and, more generally, carbon cycle studies.
Andreas Engel, Harald Bönisch, Markus Ullrich, Robert Sitals, Olivier Membrive, Francois Danis, and Cyril Crevoisier
Atmos. Chem. Phys., 17, 6825–6838, https://doi.org/10.5194/acp-17-6825-2017, https://doi.org/10.5194/acp-17-6825-2017, 2017
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AirCore is new technique for sampling stratospheric air. We present new observations of CO2 and CH4 using AirCore and derive stratospheric transport time, called the mean age of air. The purpose of using AirCore is to provide a cost-effective tool for deriving mean age. Mean age may serve as a proxy to investigate changes in stratospheric circulation. We show that there is no statistically significant trend in our 40-year time series of mean age, which is now extended using AirCore.
Malte Meinshausen, Elisabeth Vogel, Alexander Nauels, Katja Lorbacher, Nicolai Meinshausen, David M. Etheridge, Paul J. Fraser, Stephen A. Montzka, Peter J. Rayner, Cathy M. Trudinger, Paul B. Krummel, Urs Beyerle, Josep G. Canadell, John S. Daniel, Ian G. Enting, Rachel M. Law, Chris R. Lunder, Simon O'Doherty, Ron G. Prinn, Stefan Reimann, Mauro Rubino, Guus J. M. Velders, Martin K. Vollmer, Ray H. J. Wang, and Ray Weiss
Geosci. Model Dev., 10, 2057–2116, https://doi.org/10.5194/gmd-10-2057-2017, https://doi.org/10.5194/gmd-10-2057-2017, 2017
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Climate change is primarily driven by human-induced increases of greenhouse gas (GHG) concentrations. Based on ongoing community efforts (e.g. AGAGE and NOAA networks, ice cores), this study presents historical concentrations of CO2, CH4, N2O and 40 other GHGs from year 0 to year 2014. The data is recommended as input for climate models for pre-industrial, historical runs under CMIP6. Global means, but also latitudinal by monthly surface concentration fields are provided.
Peter G. Simmonds, Matthew Rigby, Archie McCulloch, Simon O'Doherty, Dickon Young, Jens Mühle, Paul B. Krummel, Paul Steele, Paul J. Fraser, Alistair J. Manning, Ray F. Weiss, Peter K. Salameh, Chris M. Harth, Ray H. J. Wang, and Ronald G. Prinn
Atmos. Chem. Phys., 17, 4641–4655, https://doi.org/10.5194/acp-17-4641-2017, https://doi.org/10.5194/acp-17-4641-2017, 2017
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This paper reports how long-term atmospheric measurements demonstrate that the Montreal Protocol has been effective in controlling production and consumption of the hydrochlorofluorocarbons, a group of industrial chemicals that have detrimental effects on the ozone layer and also contribute to global warming as greenhouse gases and their hydrofluorocarbon substitutes which are also potent greenhouse gases but do not materially affect the ozone layer.
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.
Mohamadou Diallo, Bernard Legras, Eric Ray, Andreas Engel, and Juan A. Añel
Atmos. Chem. Phys., 17, 3861–3878, https://doi.org/10.5194/acp-17-3861-2017, https://doi.org/10.5194/acp-17-3861-2017, 2017
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We construct a new monthly zonal mean CO2 distribution from the upper troposphere to the stratosphere over the 2000–2010 period. The main features of the CO2 distribution are consistent with expected variability due to the transport of long-lived trace gases by the Brewer–Dobson circulation. The method used to construct this CO2 product is unique and should be useful for model and satellite validation in the upper troposphere and stratosphere.
Jennifer Ostermöller, Harald Bönisch, Patrick Jöckel, and Andreas Engel
Atmos. Chem. Phys., 17, 3785–3797, https://doi.org/10.5194/acp-17-3785-2017, https://doi.org/10.5194/acp-17-3785-2017, 2017
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We analysed the temporal evolution of fractional release factors (FRFs) from EMAC model simulations for several halocarbons and nitrous oxide. The current formulation of FRFs yields values that depend on the tropospheric trend of the species. This is a problematic issue for the application of FRF in the calculation of steady-state quantities (e.g. ODP). Including a loss term in the calculation, we develop a new formulation of FRF and find that the time dependence can almost be compensated.
Whitney Bader, Benoît Bovy, Stephanie Conway, Kimberly Strong, Dan Smale, Alexander J. Turner, Thomas Blumenstock, Chris Boone, Martine Collaud Coen, Ancelin Coulon, Omaira Garcia, David W. T. Griffith, Frank Hase, Petra Hausmann, Nicholas Jones, Paul Krummel, Isao Murata, Isamu Morino, Hideaki Nakajima, Simon O'Doherty, Clare Paton-Walsh, John Robinson, Rodrigue Sandrin, Matthias Schneider, Christian Servais, Ralf Sussmann, and Emmanuel Mahieu
Atmos. Chem. Phys., 17, 2255–2277, https://doi.org/10.5194/acp-17-2255-2017, https://doi.org/10.5194/acp-17-2255-2017, 2017
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An increase of 0.31 ± 0.03 % year−1 of atmospheric methane is reported using 10 years of solar observations performed at 10 ground-based stations since 2005. These trend agree with a GEOS-Chem-tagged simulation that accounts for the contribution of each emission source and one sink in the total methane. The GEOS-Chem simulation shows that anthropogenic emissions from coal mining and gas and oil transport and exploration have played a major role in the increase methane since 2005.
Martyn P. Chipperfield, Qing Liang, Matthew Rigby, Ryan Hossaini, Stephen A. Montzka, Sandip Dhomse, Wuhu Feng, Ronald G. Prinn, Ray F. Weiss, Christina M. Harth, Peter K. Salameh, Jens Mühle, Simon O'Doherty, Dickon Young, Peter G. Simmonds, Paul B. Krummel, Paul J. Fraser, L. Paul Steele, James D. Happell, Robert C. Rhew, James Butler, Shari A. Yvon-Lewis, Bradley Hall, David Nance, Fred Moore, Ben R. Miller, James W. Elkins, Jeremy J. Harrison, Chris D. Boone, Elliot L. Atlas, and Emmanuel Mahieu
Atmos. Chem. Phys., 16, 15741–15754, https://doi.org/10.5194/acp-16-15741-2016, https://doi.org/10.5194/acp-16-15741-2016, 2016
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Carbon tetrachloride (CCl4) is a compound which, when released into the atmosphere, can cause depletion of the stratospheric ozone layer. Its emissions are controlled under the Montreal Protocol, and its atmospheric abundance is slowly decreasing. However, this decrease is not as fast as expected based on estimates of its emissions and its atmospheric lifetime. We have used an atmospheric model to look at the uncertainties in the CCl4 lifetime and to examine the impact on its atmospheric decay.
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.
Johannes C. Laube, Norfazrin Mohd Hanif, Patricia Martinerie, Eileen Gallacher, Paul J. Fraser, Ray Langenfelds, Carl A. M. Brenninkmeijer, Jakob Schwander, Emmanuel Witrant, Jia-Lin Wang, Chang-Feng Ou-Yang, Lauren J. Gooch, Claire E. Reeves, William T. Sturges, and David E. Oram
Atmos. Chem. Phys., 16, 15347–15358, https://doi.org/10.5194/acp-16-15347-2016, https://doi.org/10.5194/acp-16-15347-2016, 2016
Florian Obersteiner, Harald Bönisch, Timo Keber, Simon O'Doherty, and Andreas Engel
Atmos. Meas. Tech., 9, 5265–5279, https://doi.org/10.5194/amt-9-5265-2016, https://doi.org/10.5194/amt-9-5265-2016, 2016
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The analysis of trace gases in ambient air requires a preconcentration technique, in many cases to make the species of interest detectable and quantifiable. In this paper, such a preconcentration set-up is presented. Target species are trapped on adsorptive material cooled by a Stirling cooler which allows for a very low adsorption temperature but only requires electrical power. A simple and lightweight mechanical design guarantees very good suitability for remote-site field operation.
Francesco Graziosi, Jgor Arduini, Paolo Bonasoni, Francesco Furlani, Umberto Giostra, Alistair J. Manning, Archie McCulloch, Simon O'Doherty, Peter G. Simmonds, Stefan Reimann, Martin K. Vollmer, and Michela Maione
Atmos. Chem. Phys., 16, 12849–12859, https://doi.org/10.5194/acp-16-12849-2016, https://doi.org/10.5194/acp-16-12849-2016, 2016
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Carbon tetrachloride is an ozone-depleting greenhouse gas banned under the Montreal Protocol. Measurements of atmospheric levels combined with global transport models indicate that it is still being emitted, in contrast to what is reported. In order to help solve the "mystery of carbon tetrachloride", we estimated European emissions during 2006–2014 using atmospheric observations and models. We identified emission hot spots and showed inconsistencies in national emission declarations.
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.
Cathy M. Trudinger, Paul J. Fraser, David M. Etheridge, William T. Sturges, Martin K. Vollmer, Matt Rigby, Patricia Martinerie, Jens Mühle, David R. Worton, Paul B. Krummel, L. Paul Steele, Benjamin R. Miller, Johannes Laube, Francis S. Mani, Peter J. Rayner, Christina M. Harth, Emmanuel Witrant, Thomas Blunier, Jakob Schwander, Simon O'Doherty, and Mark Battle
Atmos. Chem. Phys., 16, 11733–11754, https://doi.org/10.5194/acp-16-11733-2016, https://doi.org/10.5194/acp-16-11733-2016, 2016
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Perfluorocarbons (PFCs) are potent, long-lived and mostly man-made greenhouse gases released to the atmosphere mainly during aluminium production and semiconductor manufacture. Here we present the first continuous histories of three PFCs from 1800 to 2014, derived from measurements of these PFCs in the atmosphere and in air bubbles in polar ice. The records show how human actions have affected these important greenhouse gases over the past century.
Mark F. Lunt, Matt Rigby, Anita L. Ganesan, and Alistair J. Manning
Geosci. Model Dev., 9, 3213–3229, https://doi.org/10.5194/gmd-9-3213-2016, https://doi.org/10.5194/gmd-9-3213-2016, 2016
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Bayesian inversions can be used to estimate emissions of gases from atmospheric data. We present an inversion framework that objectively defines the basis functions, which describe regions of emissions. The framework allows for the uncertainty in the choice of basis functions to be propagated through to the posterior emissions distribution in a single-step process, and provides an alternative to using a single set of basis functions.
Stefan Müller, Peter Hoor, Heiko Bozem, Ellen Gute, Bärbel Vogel, Andreas Zahn, Harald Bönisch, Timo Keber, Martina Krämer, Christian Rolf, Martin Riese, Hans Schlager, and Andreas Engel
Atmos. Chem. Phys., 16, 10573–10589, https://doi.org/10.5194/acp-16-10573-2016, https://doi.org/10.5194/acp-16-10573-2016, 2016
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In situ airborne measurements performed during TACTS/ESMVal 2012 were analysed to investigate the chemical compostion of the upper troposphere and lower stratosphere. N2O, CO and O3 data show an increase in tropospherically affected air masses within the extratropical stratosphere from August to September 2012, which originate from the Asian monsoon region. Thus, the Asian monsoon anticyclone significantly affected the chemical composition of the extratropical stratosphere during summer 2012.
E. Eckert, A. Laeng, S. Lossow, S. Kellmann, G. Stiller, T. von Clarmann, N. Glatthor, M. Höpfner, M. Kiefer, H. Oelhaf, J. Orphal, B. Funke, U. Grabowski, F. Haenel, A. Linden, G. Wetzel, W. Woiwode, P. F. Bernath, C. Boone, G. S. Dutton, J. W. Elkins, A. Engel, J. C. Gille, F. Kolonjari, T. Sugita, G. C. Toon, and K. A. Walker
Atmos. Meas. Tech., 9, 3355–3389, https://doi.org/10.5194/amt-9-3355-2016, https://doi.org/10.5194/amt-9-3355-2016, 2016
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We investigate the accuracy, precision and long-term stability of the MIPAS Envisat IMK/IAA CFC-11 (CCl3F) and CFC-12 (CCl2F2) products.
For comparisons we use several data products from satellite, airplane and balloon-borne instruments as well as ground-based data.
MIPAS Envisat CFC-11 has a slight high bias at the lower end of the profile.
CFC-12 agrees well with other data products.
The temporal stability is good up to ~ 30 km, but still leaves room for improvement.
R. Hossaini, P. K. Patra, A. A. Leeson, G. Krysztofiak, N. L. Abraham, S. J. Andrews, A. T. Archibald, J. Aschmann, E. L. Atlas, D. A. Belikov, H. Bönisch, L. J. Carpenter, S. Dhomse, M. Dorf, A. Engel, W. Feng, S. Fuhlbrügge, P. T. Griffiths, N. R. P. Harris, R. Hommel, T. Keber, K. Krüger, S. T. Lennartz, S. Maksyutov, H. Mantle, G. P. Mills, B. Miller, S. A. Montzka, F. Moore, M. A. Navarro, D. E. Oram, K. Pfeilsticker, J. A. Pyle, B. Quack, A. D. Robinson, E. Saikawa, A. Saiz-Lopez, S. Sala, B.-M. Sinnhuber, S. Taguchi, S. Tegtmeier, R. T. Lidster, C. Wilson, and F. Ziska
Atmos. Chem. Phys., 16, 9163–9187, https://doi.org/10.5194/acp-16-9163-2016, https://doi.org/10.5194/acp-16-9163-2016, 2016
Joe McNorton, Martyn P. Chipperfield, Manuel Gloor, Chris Wilson, Wuhu Feng, Garry D. Hayman, Matt Rigby, Paul B. Krummel, Simon O'Doherty, Ronald G. Prinn, Ray F. Weiss, Dickon Young, Ed Dlugokencky, and Steve A. Montzka
Atmos. Chem. Phys., 16, 7943–7956, https://doi.org/10.5194/acp-16-7943-2016, https://doi.org/10.5194/acp-16-7943-2016, 2016
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Methane (CH4) is an important greenhouse gas. The growth of atmospheric CH4 stalled from 1999 to 2006, with current explanations focussed mainly on changing surface fluxes. We combine models with observations and meteorological data to assess the atmospheric contribution to CH4 changes. We find that variations in mean atmospheric hydroxyl concentration can explain part of the stall in growth. Our study highlights the role of multi-annual variability in atmospheric chemistry in global CH4 trends.
Armin Rauthe-Schöch, Angela K. Baker, Tanja J. Schuck, Carl A. M. Brenninkmeijer, Andreas Zahn, Markus Hermann, Greta Stratmann, Helmut Ziereis, Peter F. J. van Velthoven, and Jos Lelieveld
Atmos. Chem. Phys., 16, 3609–3629, https://doi.org/10.5194/acp-16-3609-2016, https://doi.org/10.5194/acp-16-3609-2016, 2016
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The flying laboratory CARIBIC onboard a passenger aircraft measured trace gases and aerosol particles in the upper tropospheric Indian summer monsoon anticyclone in summer 2008. We used the measurements together with meteorological analyses to investigate the chemical signature of the northern and southern part of the monsoon, the source regions from where the air was entrained into the monsoon and which parts of the world received polluted air that had been chemically processed in the monsoon.
M. Chirkov, G. P. Stiller, A. Laeng, S. Kellmann, T. von Clarmann, C. D. Boone, J. W. Elkins, A. Engel, N. Glatthor, U. Grabowski, C. M. Harth, M. Kiefer, F. Kolonjari, P. B. Krummel, A. Linden, C. R. Lunder, B. R. Miller, S. A. Montzka, J. Mühle, S. O'Doherty, J. Orphal, R. G. Prinn, G. Toon, M. K. Vollmer, K. A. Walker, R. F. Weiss, A. Wiegele, and D. Young
Atmos. Chem. Phys., 16, 3345–3368, https://doi.org/10.5194/acp-16-3345-2016, https://doi.org/10.5194/acp-16-3345-2016, 2016
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HCFC-22 global distributions from MIPAS measurements for 2005 to 2012 are presented. Tropospheric trends are in good agreement with ground-based observations. A layer of enhanced HCFC-22 in the upper tropospheric tropics and northern subtropics is identified to come from Asian sources uplifted in the Asian monsoon. Stratospheric distributions provide show seasonal, semi-annual, and QBO-related variations. Hemispheric asymmetries of trends hint towards a change in the stratospheric circulation.
Andreas Engel, Harald Bönisch, Tim Schwarzenberger, Hans-Peter Haase, Katja Grunow, Jana Abalichin, and Stephan Sala
Atmos. Meas. Tech., 9, 1051–1062, https://doi.org/10.5194/amt-9-1051-2016, https://doi.org/10.5194/amt-9-1051-2016, 2016
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We present a validation of MIPAS-ENVISAT vertical profiles (ESA operational retrieval version 6.0) of N2O, CH4, CFC-12, and CFC-11. The geophysical validation is performed using data from a balloon-borne cryogenic whole air sampler and trajectory matching. We show that the validation results are different for the period prior to 2005 compared to the post 2005 period. N2O, CH4, and CFC-12 show partly good agreement while CFC-11 data from this retrieval cannot be used for scientific studies.
Stig B. Dalsøren, Cathrine L. Myhre, Gunnar Myhre, Angel J. Gomez-Pelaez, Ole A. Søvde, Ivar S. A. Isaksen, Ray F. Weiss, and Christina M. Harth
Atmos. Chem. Phys., 16, 3099–3126, https://doi.org/10.5194/acp-16-3099-2016, https://doi.org/10.5194/acp-16-3099-2016, 2016
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Methane is a key greenhouse gas. Observations at surface sites show a more than 10 % increase over the period 1984–2012. Using an atmospheric model we calculate a growth in the atmospheric chemical methane loss the last decades. Without this, the rise in atmospheric methane would have been even higher. The model reproduces trends and short-term variations in observation data. However, some discrepancies in model performance question the accuracy in estimates of emission increases in Asia.
F. Obersteiner, H. Bönisch, and A. Engel
Atmos. Meas. Tech., 9, 179–194, https://doi.org/10.5194/amt-9-179-2016, https://doi.org/10.5194/amt-9-179-2016, 2016
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We present the characterization and application of a new gas chromatography time-of-flight mass spectrometry instrument, with focus on quantitative analysis of halocarbons in air samples. The applicability of the TOFMS technique, e.g. to form the basis of a "digital air archieve", is supported by the findings of this work: very high sensitivity, high measurement precision, a large dynamical range and an open data format which allows in-depth analysis of the data.
P. G. Simmonds, M. Rigby, A. J. Manning, M. F. Lunt, S. O'Doherty, A. McCulloch, P. J. Fraser, S. Henne, M. K. Vollmer, J. Mühle, R. F. Weiss, P. K. Salameh, D. Young, S. Reimann, A. Wenger, T. Arnold, C. M. Harth, P. B. Krummel, L. P. Steele, B. L. Dunse, B. R. Miller, C. R. Lunder, O. Hermansen, N. Schmidbauer, T. Saito, Y. Yokouchi, S. Park, S. Li, B. Yao, L. X. Zhou, J. Arduini, M. Maione, R. H. J. Wang, D. Ivy, and R. G. Prinn
Atmos. Chem. Phys., 16, 365–382, https://doi.org/10.5194/acp-16-365-2016, https://doi.org/10.5194/acp-16-365-2016, 2016
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We report regional and global emissions estimates of HFC-152a using high frequency measurements from 11 observing sites and archived air samples dating back to 1978 together with atmospheric transport models. The "bottom-up" emissions of HFC-152a reported to the UNFCCC appear to significantly underestimate those reported here from observations. This discrepancy we suggest arises from largely underestimated USA and undeclared Asian emissions.
A. Laeng, J. Plieninger, T. von Clarmann, U. Grabowski, G. Stiller, E. Eckert, N. Glatthor, F. Haenel, S. Kellmann, M. Kiefer, A. Linden, S. Lossow, L. Deaver, A. Engel, M. Hervig, I. Levin, M. McHugh, S. Noël, G. Toon, and K. Walker
Atmos. Meas. Tech., 8, 5251–5261, https://doi.org/10.5194/amt-8-5251-2015, https://doi.org/10.5194/amt-8-5251-2015, 2015
S. J. Lawson, M. D. Keywood, I. E. Galbally, J. L. Gras, J. M. Cainey, M. E. Cope, P. B. Krummel, P. J. Fraser, L. P. Steele, S. T. Bentley, C. P. Meyer, Z. Ristovski, and A. H. Goldstein
Atmos. Chem. Phys., 15, 13393–13411, https://doi.org/10.5194/acp-15-13393-2015, https://doi.org/10.5194/acp-15-13393-2015, 2015
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Biomass burning (BB) plumes were opportunistically measured at the Cape Grim Baseline Station in Tasmania, Australia. We provide a unique set of trace gas and particle emission factors for temperate Australian coastal heathland fires, and attribute a major short-lived enhancement in emission ratios to a minor rainfall event. The ability of BB particles to act as cloud condensation nuclei, and the contribution of BB emissions to observed particle growth and ozone enhancements are discussed.
M. K. Kajos, P. Rantala, M. Hill, H. Hellén, J. Aalto, J. Patokoski, R. Taipale, C. C. Hoerger, S. Reimann, T. M. Ruuskanen, J. Rinne, and T. Petäjä
Atmos. Meas. Tech., 8, 4453–4473, https://doi.org/10.5194/amt-8-4453-2015, https://doi.org/10.5194/amt-8-4453-2015, 2015
K. C. Wells, D. B. Millet, N. Bousserez, D. K. Henze, S. Chaliyakunnel, T. J. Griffis, Y. Luan, E. J. Dlugokencky, R. G. Prinn, S. O'Doherty, R. F. Weiss, G. S. Dutton, J. W. Elkins, P. B. Krummel, R. Langenfelds, L. P. Steele, E. A. Kort, S. C. Wofsy, and T. Umezawa
Geosci. Model Dev., 8, 3179–3198, https://doi.org/10.5194/gmd-8-3179-2015, https://doi.org/10.5194/gmd-8-3179-2015, 2015
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This paper introduces a new inversion framework for N2O using GEOS-Chem and its adjoint, which we employed in a series of observing system simulation experiments to evaluate the source and sink constraints provided by surface and aircraft-based N2O measurements. We also applied a new approach for estimating a posteriori uncertainty for high-dimensional inversions, and used it to quantify the spatial and temporal resolution of N2O emission constraints achieved with the current observing network.
C. C. Hoerger, A. Claude, C. Plass-Duelmer, S. Reimann, E. Eckart, R. Steinbrecher, J. Aalto, J. Arduini, N. Bonnaire, J. N. Cape, A. Colomb, R. Connolly, J. Diskova, P. Dumitrean, C. Ehlers, V. Gros, H. Hakola, M. Hill, J. R. Hopkins, J. Jäger, R. Junek, M. K. Kajos, D. Klemp, M. Leuchner, A. C. Lewis, N. Locoge, M. Maione, D. Martin, K. Michl, E. Nemitz, S. O'Doherty, P. Pérez Ballesta, T. M. Ruuskanen, S. Sauvage, N. Schmidbauer, T. G. Spain, E. Straube, M. Vana, M. K. Vollmer, R. Wegener, and A. Wenger
Atmos. Meas. Tech., 8, 2715–2736, https://doi.org/10.5194/amt-8-2715-2015, https://doi.org/10.5194/amt-8-2715-2015, 2015
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The performance of 20 European laboratories involved in long-term non-methane hydrocarbon (NMHC) measurements was assessed with respect to ACTRIS and GAW data quality objectives. The participants were asked to measure both a 30-component NMHC mixture in nitrogen and whole air. The NMHCs were analysed either by GC-FID or GC-MS. Most systems performed well for the NMHC in nitrogen, whereas in air more scatter was observed. Reasons for this are explained in the paper.
A. L. Ganesan, A. J. Manning, A. Grant, D. Young, D .E. Oram, W. T. Sturges, J. B. Moncrieff, and S. O'Doherty
Atmos. Chem. Phys., 15, 6393–6406, https://doi.org/10.5194/acp-15-6393-2015, https://doi.org/10.5194/acp-15-6393-2015, 2015
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The UK is one of several countries to enact legislation to reduce its greenhouse gas emissions. We present top-down emissions of methane and nitrous oxide for the UK and Ireland over 2012-2014. We inferred average UK emissions of 2.09Tg/yr CH4 and 0.101Tg/yr N2O and used sectoral distributions to determine whether these discrepancies can be attributed to specific source sectors. We found the agricultural sector likely to be overestimated in the bottom-up emissions inventories of both gases.
J. Hoker, F. Obersteiner, H. Bönisch, and A. Engel
Atmos. Meas. Tech., 8, 2195–2206, https://doi.org/10.5194/amt-8-2195-2015, https://doi.org/10.5194/amt-8-2195-2015, 2015
J. A. Fisher, S. R. Wilson, G. Zeng, J. E. Williams, L. K. Emmons, R. L. Langenfelds, P. B. Krummel, and L. P. Steele
Atmos. Chem. Phys., 15, 3217–3239, https://doi.org/10.5194/acp-15-3217-2015, https://doi.org/10.5194/acp-15-3217-2015, 2015
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The Southern Hemisphere (SH) serves as an important test bed for evaluating our understanding of the processes that drive the composition of the clean background atmosphere. Using data from two aircraft campaigns, combined with four atmospheric chemistry models, we find a large sensitivity in the remote SH to biogenic emissions and their subsequent chemistry and transport. Future model evaluation and measurement campaigns should prioritize reducing uncertainties in these processes.
A. Ghosh, P. K. Patra, K. Ishijima, T. Umezawa, A. Ito, D. M. Etheridge, S. Sugawara, K. Kawamura, J. B. Miller, E. J. Dlugokencky, P. B. Krummel, P. J. Fraser, L. P. Steele, R. L. Langenfelds, C. M. Trudinger, J. W. C. White, B. Vaughn, T. Saeki, S. Aoki, and T. Nakazawa
Atmos. Chem. Phys., 15, 2595–2612, https://doi.org/10.5194/acp-15-2595-2015, https://doi.org/10.5194/acp-15-2595-2015, 2015
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Atmospheric CH4 increased from 900ppb to 1800ppb during the period 1900–2010 at a rate unprecedented in any observational records. We use bottom-up emissions and a chemistry-transport model to simulate CH4. The optimized global total CH4 emission, estimated from the model–observation differences, increased at fastest rate during 1940–1990. Using δ13C of CH4 measurements we attribute this emission increase to biomass burning. Total CH4 lifetime is shortened by 4% over the simulation period.
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
Z. M. Loh, R. M. Law, K. D. Haynes, P. B. Krummel, L. P. Steele, P. J. Fraser, S. D. Chambers, and A. G. Williams
Atmos. Chem. Phys., 15, 305–317, https://doi.org/10.5194/acp-15-305-2015, https://doi.org/10.5194/acp-15-305-2015, 2015
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The paper compares methane observations at Cape Grim, Tasmania, with model-simulated methane to better constrain methane fluxes from southeastern Australia. Inventory estimates of anthropogenic methane emissions appear to be supported by observed atmospheric methane. A missing methane source in springtime (October to November) is tentatively attributed to wetland emissions.
M. Kaufmann, J. Blank, T. Guggenmoser, J. Ungermann, A. Engel, M. Ern, F. Friedl-Vallon, D. Gerber, J. U. Grooß, G. Guenther, M. Höpfner, A. Kleinert, E. Kretschmer, Th. Latzko, G. Maucher, T. Neubert, H. Nordmeyer, H. Oelhaf, F. Olschewski, J. Orphal, P. Preusse, H. Schlager, H. Schneider, D. Schuettemeyer, F. Stroh, O. Suminska-Ebersoldt, B. Vogel, C. M. Volk, W. Woiwode, and M. Riese
Atmos. Meas. Tech., 8, 81–95, https://doi.org/10.5194/amt-8-81-2015, https://doi.org/10.5194/amt-8-81-2015, 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.
A. Fraser, P. I. Palmer, L. Feng, H. Bösch, R. Parker, E. J. Dlugokencky, P. B. Krummel, and R. L. Langenfelds
Atmos. Chem. Phys., 14, 12883–12895, https://doi.org/10.5194/acp-14-12883-2014, https://doi.org/10.5194/acp-14-12883-2014, 2014
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Satellite measurements of CO2 and CH4 can be subject to regional systematic errors that can consequently compromise their ability to infer robust flux estimates of these two gases. We develop a method to use retrieved ratios of CH4 and CO2 that are less affected by systematic error. We show that additional in situ data are needed to anchor these observed ratios so they can simultaneously infer fluxes of CO2 and CH4. We argue the ratio data will provide a more faithful description of true fluxes.
W. Bader, T. Stavrakou, J.-F. Muller, S. Reimann, C. D. Boone, J. J. Harrison, O. Flock, B. Bovy, B. Franco, B. Lejeune, C. Servais, and E. Mahieu
Atmos. Meas. Tech., 7, 3861–3872, https://doi.org/10.5194/amt-7-3861-2014, https://doi.org/10.5194/amt-7-3861-2014, 2014
M. Maione, F. Graziosi, J. Arduini, F. Furlani, U. Giostra, D. R. Blake, P. Bonasoni, X. Fang, S. A. Montzka, S. J. O'Doherty, S. Reimann, A. Stohl, and M. K. Vollmer
Atmos. Chem. Phys., 14, 9755–9770, https://doi.org/10.5194/acp-14-9755-2014, https://doi.org/10.5194/acp-14-9755-2014, 2014
S. O'Doherty, M. Rigby, J. Mühle, D. J. Ivy, B. R. Miller, D. Young, P. G. Simmonds, S. Reimann, M. K. Vollmer, P. B. Krummel, P. J. Fraser, L. P. Steele, B. Dunse, P. K. Salameh, C. M. Harth, T. Arnold, R. F. Weiss, J. Kim, S. Park, S. Li, C. Lunder, O. Hermansen, N. Schmidbauer, L. X. Zhou, B. Yao, R. H. J. Wang, A. J. Manning, and R. G. Prinn
Atmos. Chem. Phys., 14, 9249–9258, https://doi.org/10.5194/acp-14-9249-2014, https://doi.org/10.5194/acp-14-9249-2014, 2014
A. Tilgner, L. Schöne, P. Bräuer, D. van Pinxteren, E. Hoffmann, G. Spindler, S. A. Styler, S. Mertes, W. Birmili, R. Otto, M. Merkel, K. Weinhold, A. Wiedensohler, H. Deneke, R. Schrödner, R. Wolke, J. Schneider, W. Haunold, A. Engel, A. Wéber, and H. Herrmann
Atmos. Chem. Phys., 14, 9105–9128, https://doi.org/10.5194/acp-14-9105-2014, https://doi.org/10.5194/acp-14-9105-2014, 2014
S. N. Vardag, S. Hammer, S. O'Doherty, T. G. Spain, B. Wastine, A. Jordan, and I. Levin
Atmos. Chem. Phys., 14, 8403–8418, https://doi.org/10.5194/acp-14-8403-2014, https://doi.org/10.5194/acp-14-8403-2014, 2014
S. Sala, H. Bönisch, T. Keber, D. E. Oram, G. Mills, and A. Engel
Atmos. Chem. Phys., 14, 6903–6923, https://doi.org/10.5194/acp-14-6903-2014, https://doi.org/10.5194/acp-14-6903-2014, 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
E. Saikawa, R. G. Prinn, E. Dlugokencky, K. Ishijima, G. S. Dutton, B. D. Hall, R. Langenfelds, Y. Tohjima, T. Machida, M. Manizza, M. Rigby, S. O'Doherty, P. K. Patra, C. M. Harth, R. F. Weiss, P. B. Krummel, M. van der Schoot, P. J. Fraser, L. P. Steele, S. Aoki, T. Nakazawa, and J. W. Elkins
Atmos. Chem. Phys., 14, 4617–4641, https://doi.org/10.5194/acp-14-4617-2014, https://doi.org/10.5194/acp-14-4617-2014, 2014
R. L. Thompson, P. K. Patra, K. Ishijima, E. Saikawa, M. Corazza, U. Karstens, C. Wilson, P. Bergamaschi, E. Dlugokencky, C. Sweeney, R. G. Prinn, R. F. Weiss, S. O'Doherty, P. J. Fraser, L. P. Steele, P. B. Krummel, M. Saunois, M. Chipperfield, and P. Bousquet
Atmos. Chem. Phys., 14, 4349–4368, https://doi.org/10.5194/acp-14-4349-2014, https://doi.org/10.5194/acp-14-4349-2014, 2014
A. L. Ganesan, M. Rigby, A. Zammit-Mangion, A. J. Manning, R. G. Prinn, P. J. Fraser, C. M. Harth, K.-R. Kim, P. B. Krummel, S. Li, J. Mühle, S. J. O'Doherty, S. Park, P. K. Salameh, L. P. Steele, and R. F. Weiss
Atmos. Chem. Phys., 14, 3855–3864, https://doi.org/10.5194/acp-14-3855-2014, https://doi.org/10.5194/acp-14-3855-2014, 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
C. Dyroff, A. Zahn, S. Sanati, E. Christner, A. Rauthe-Schöch, and T. J. Schuck
Atmos. Meas. Tech., 7, 743–755, https://doi.org/10.5194/amt-7-743-2014, https://doi.org/10.5194/amt-7-743-2014, 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
R. L. Thompson, F. Chevallier, A. M. Crotwell, G. Dutton, R. L. Langenfelds, R. G. Prinn, R. F. Weiss, Y. Tohjima, T. Nakazawa, P. B. Krummel, L. P. Steele, P. Fraser, S. O'Doherty, K. Ishijima, and S. Aoki
Atmos. Chem. Phys., 14, 1801–1817, https://doi.org/10.5194/acp-14-1801-2014, https://doi.org/10.5194/acp-14-1801-2014, 2014
B. D. Hall, A. Engel, J. Mühle, J. W. Elkins, F. Artuso, E. Atlas, M. Aydin, D. Blake, E.-G. Brunke, S. Chiavarini, P. J. Fraser, J. Happell, P. B. Krummel, I. Levin, M. Loewenstein, M. Maione, S. A. Montzka, S. O'Doherty, S. Reimann, G. Rhoderick, E. S. Saltzman, H. E. Scheel, L. P. Steele, M. K. Vollmer, R. F. Weiss, D. Worthy, and Y. Yokouchi
Atmos. Meas. Tech., 7, 469–490, https://doi.org/10.5194/amt-7-469-2014, https://doi.org/10.5194/amt-7-469-2014, 2014
E. Mahieu, R. Zander, G. C. Toon, M. K. Vollmer, S. Reimann, J. Mühle, W. Bader, B. Bovy, B. Lejeune, C. Servais, P. Demoulin, G. Roland, P. F. Bernath, C. D. Boone, K. A. Walker, and P. Duchatelet
Atmos. Meas. Tech., 7, 333–344, https://doi.org/10.5194/amt-7-333-2014, https://doi.org/10.5194/amt-7-333-2014, 2014
M. J. Ashfold, N. R. P. Harris, A. J. Manning, A. D. Robinson, N. J. Warwick, and J. A. Pyle
Atmos. Chem. Phys., 14, 979–994, https://doi.org/10.5194/acp-14-979-2014, https://doi.org/10.5194/acp-14-979-2014, 2014
C. Cressot, F. Chevallier, P. Bousquet, C. Crevoisier, E. J. Dlugokencky, A. Fortems-Cheiney, C. Frankenberg, R. Parker, I. Pison, R. A. Scheepmaker, S. A. Montzka, P. B. Krummel, L. P. Steele, and R. L. Langenfelds
Atmos. Chem. Phys., 14, 577–592, https://doi.org/10.5194/acp-14-577-2014, https://doi.org/10.5194/acp-14-577-2014, 2014
S. Tegtmeier, K. Krüger, B. Quack, E. Atlas, D. R. Blake, H. Boenisch, A. Engel, H. Hepach, R. Hossaini, M. A. Navarro, S. Raimund, S. Sala, Q. Shi, and F. Ziska
Atmos. Chem. Phys., 13, 11869–11886, https://doi.org/10.5194/acp-13-11869-2013, https://doi.org/10.5194/acp-13-11869-2013, 2013
R. Hossaini, H. Mantle, M. P. Chipperfield, S. A. Montzka, P. Hamer, F. Ziska, B. Quack, K. Krüger, S. Tegtmeier, E. Atlas, S. Sala, A. Engel, H. Bönisch, T. Keber, D. Oram, G. Mills, C. Ordóñez, A. Saiz-Lopez, N. Warwick, Q. Liang, W. Feng, F. Moore, B. R. Miller, V. Marécal, N. A. D. Richards, M. Dorf, and K. Pfeilsticker
Atmos. Chem. Phys., 13, 11819–11838, https://doi.org/10.5194/acp-13-11819-2013, https://doi.org/10.5194/acp-13-11819-2013, 2013
A. L. Ganesan, A. Chatterjee, R. G. Prinn, C. M. Harth, P. K. Salameh, A. J. Manning, B. D. Hall, J. Mühle, L. K. Meredith, R. F. Weiss, S. O'Doherty, and D. Young
Atmos. Chem. Phys., 13, 10633–10644, https://doi.org/10.5194/acp-13-10633-2013, https://doi.org/10.5194/acp-13-10633-2013, 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. D. Hamer, V. Marécal, R. Hossaini, M. Pirre, N. Warwick, M. Chipperfield, A. A. Samah, N. Harris, A. Robinson, B. Quack, A. Engel, K. Krüger, E. Atlas, K. Subramaniam, D. Oram, Emma C. Leedham Elvidge, G. Mills, K. Pfeilsticker, S. Sala, T. Keber, H. Bönisch, L. K. Peng, M. S. M. Nadzir, P. T. Lim, A. Mujahid, A. Anton, H. Schlager, V. Catoire, G. Krysztofiak, S. Fühlbrügge, M. Dorf, and W. T. Sturges
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-13-20611-2013, https://doi.org/10.5194/acpd-13-20611-2013, 2013
Revised manuscript not accepted
A. Fraser, P. I. Palmer, L. Feng, H. Boesch, A. Cogan, R. Parker, E. J. Dlugokencky, P. J. Fraser, P. B. Krummel, R. L. Langenfelds, S. O'Doherty, R. G. Prinn, L. P. Steele, M. van der Schoot, and R. F. Weiss
Atmos. Chem. Phys., 13, 5697–5713, https://doi.org/10.5194/acp-13-5697-2013, https://doi.org/10.5194/acp-13-5697-2013, 2013
L. R. Welp, R. F. Keeling, R. F. Weiss, W. Paplawsky, and S. Heckman
Atmos. Meas. Tech., 6, 1217–1226, https://doi.org/10.5194/amt-6-1217-2013, https://doi.org/10.5194/amt-6-1217-2013, 2013
C. Crevoisier, D. Nobileau, R. Armante, L. Crépeau, T. Machida, Y. Sawa, H. Matsueda, T. Schuck, T. Thonat, J. Pernin, N. A. Scott, and A. Chédin
Atmos. Chem. Phys., 13, 4279–4289, https://doi.org/10.5194/acp-13-4279-2013, https://doi.org/10.5194/acp-13-4279-2013, 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
C. E. Yver, H. D. Graven, D. D. Lucas, P. J. Cameron-Smith, R. F. Keeling, and R. F. Weiss
Atmos. Chem. Phys., 13, 1837–1852, https://doi.org/10.5194/acp-13-1837-2013, https://doi.org/10.5194/acp-13-1837-2013, 2013
C. M. Trudinger, I. G. Enting, P. J. Rayner, D. M. Etheridge, C. Buizert, M. Rubino, P. B. Krummel, and T. Blunier
Atmos. Chem. Phys., 13, 1485–1510, https://doi.org/10.5194/acp-13-1485-2013, https://doi.org/10.5194/acp-13-1485-2013, 2013
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Physics (physical properties and processes)
Distinct structures of interannual variations in stratosphere-to-troposphere ozone transport induced by the Tibetan Plateau thermal forcing
Global CH4 fluxes derived from JAXA/GOSAT lower-tropospheric partial column data and the CarbonTracker Europe-CH4 atmospheric inverse model
Improved understanding of anthropogenic and biogenic carbonyl sulfide (COS) fluxes in western Europe from long-term continuous mixing ratio measurements
The skill at modeling an extremely high ozone episode varies substantially amongst ensemble simulation
Quantifying transboundary transport flux of CO over the Tibetan Plateau: variabilities and drivers
Inverse modelling of New Zealand's carbon dioxide balance estimates a larger than expected carbon sink
Combined CO2 measurement record indicates Amazon forest carbon uptake is offset by savanna carbon release
Operational and Probabilistic Evaluation of AQMEII-4 Regional Scale Ozone Dry Deposition. Time to Harmonise Our LULC Masks
The importance of moist thermodynamics on neutral buoyancy height for plumes from anthropogenic sources
Partitioning anthropogenic and natural methane emissions in Finland during 2000–2021 by combining bottom-up and top-down estimates
A Diagnostic Intercomparison of Modeled Ozone Dry Deposition Over North America and Europe Using AQMEII4 Regional-Scale Simulations
The role of OCO-3 XCO2 retrievals in estimating global terrestrial net ecosystem exchanges
Surface and tropospheric ozone over East Asia and Southeast Asia from observations: distributions, trends, and variability
The improved Trajectory-mapped Ozonesonde dataset for the Stratosphere and Troposphere (TOST): update, validation and applications
Constraining elemental mercury air–sea exchange using long-term ground-based observations
Climate Forcing due to Future Ozone Changes: An intercomparison of metrics and methods
Variation in shortwave water vapour continuum and impact on clear-sky shortwave radiative feedback
Tracing the origins of stratospheric ozone intrusions: direct vs. indirect pathways and their impacts on Central and Eastern China in spring–summer 2019
Flow-dependent observation errors for greenhouse gas inversions in an ensemble Kalman smoother
A WRF-Chem study of the greenhouse gas column and in situ surface concentrations observed at Xianghe, China. Part 1: Methane (CH4)
Evaluation and updates to the oxidized reactive nitrogen trace gas dry deposition parameterization from the GEOS-Chem CTM, including a pathway for ground surface NO2 hydrolysis
Observational and model evidence for a prominent stratospheric influence on variability in tropospheric nitrous oxide
Estimation of Canada's methane emissions: inverse modelling analysis using the Environment and Climate Change Canada (ECCC) measurement network
Spatiotemporal source apportionment of ozone pollution over the Greater Bay Area
Potential of 14C-based vs. ΔCO-based ΔffCO2 observations to estimate urban fossil fuel CO2 (ffCO2) emissions
On the uncertainty of anthropogenic aromatic volatile organic compound emissions: model evaluation and sensitivity analysis
A mechanism of stratospheric O3 intrusion into the atmospheric environment: a case study of the North China Plain
Influence of atmospheric circulation on the interannual variability of transport from global and regional emissions into the Arctic
Surface networks in the Arctic may miss a future methane bomb
Potential of using CO2 observations over India in a regional carbon budget estimation by improving the modelling system
A bottom-up emission estimate for the 2022 Nord Stream gas leak: derivation, simulations, and evaluation
European CH4 inversions with ICON-ART coupled to the CarbonTracker Data Assimilation Shell
Extreme weather exacerbates ozone pollution in the Pearl River Delta, China: role of natural processes
Multidecadal ozone trends in China and implications for human health and crop yields: a hybrid approach combining a chemical transport model and machine learning
On the influence of vertical mixing, boundary layer schemes, and temporal emission profiles on tropospheric NO2 in WRF-Chem – comparisons to in situ, satellite, and MAX-DOAS observations
Decreasing trends of ammonia emissions over Europe seen from remote sensing and inverse modelling
The sensitivity of Southern Ocean atmospheric dimethyl sulfide (DMS) to modeled oceanic DMS concentrations and emissions
Impacts of maritime shipping on air pollution along the US East Coast
Understanding greenhouse gas (GHG) column concentrations in Munich using the Weather Research and Forecasting (WRF) model
Impact of transport model resolution and a priori assumptions on inverse modeling of Swiss F-gas emissions
Estimation of power plant SO2 emissions using the HYSPLIT dispersion model and airborne observations with plume rise ensemble runs
Can we use atmospheric CO2 measurements to verify emission trends reported by cities? Lessons from a 6-year atmospheric inversion over Paris
A new steady-state gas–particle partitioning model of polycyclic aromatic hydrocarbons: implication for the influence of the particulate proportion in emissions
An analysis of CMAQ gas-phase dry deposition over North America through grid-scale and land-use-specific diagnostics in the context of AQMEII4
Rethinking the role of transport and photochemistry in regional ozone pollution: insights from ozone concentration and mass budgets
Decreasing seasonal cycle amplitude of methane in the northern high latitudes being driven by lower-latitude changes in emissions and transport
The effect of anthropogenic emission, meteorological factors, and carbon dioxide on the surface ozone increase in China from 2008 to 2018 during the East Asia summer monsoon season
Development of a CMAQ–PMF-based composite index for prescribing an effective ozone abatement strategy: a case study of sensitivity of surface ozone to precursor volatile organic compound species in southern Taiwan
Comment on “Climate consequences of hydrogen emissions” by Ocko and Hamburg (2022)
Constraining emissions of volatile organic compounds from western US wildfires with WE-CAN and FIREX-AQ airborne observations
Qingjian Yang, Tianliang Zhao, Yongqing Bai, Kai Meng, Yuehan Luo, Zhijie Tian, Xiaoyun Sun, Weikang Fu, Kai Yang, and Jun Hu
Atmos. Chem. Phys., 25, 8029–8042, https://doi.org/10.5194/acp-25-8029-2025, https://doi.org/10.5194/acp-25-8029-2025, 2025
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This study reveals a unique driver of the Tibetan Plateau (TP) thermal forcing of the interannual variations in stratosphere-to-troposphere transport (STT) of ozone with diverse structures. Anomalous strong TP thermal forcing induces anticyclonic anomalies in the upper troposphere over the TP, which strengthens and attenuates the northern and southern branches of the westerly jet, intensifying (weakening) the westerly trough for more (fewer) tropopause folds of ozone STT over the East Asian region.
Aki Tsuruta, Akihiko Kuze, Kei Shiomi, Fumie Kataoka, Nobuhiro Kikuchi, Tuula Aalto, Leif Backman, Ella Kivimäki, Maria K. Tenkanen, Kathryn McKain, Omaira E. García, Frank Hase, Rigel Kivi, Isamu Morino, Hirofumi Ohyama, David F. Pollard, Mahesh K. Sha, Kimberly Strong, Ralf Sussmann, Yao Te, Voltaire A. Velazco, Mihalis Vrekoussis, Thorsten Warneke, Minqiang Zhou, and Hiroshi Suto
Atmos. Chem. Phys., 25, 7829–7862, https://doi.org/10.5194/acp-25-7829-2025, https://doi.org/10.5194/acp-25-7829-2025, 2025
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Satellite data bring invaluable information about greenhouse gas emissions globally. We found that a new type of data from the Greenhouse Gas Observing Satellite (GOSAT), which contains information about methane in the lowest layer of Earth's atmosphere, could provide reliable estimates of recent methane emissions when combined with atmospheric modelling. Therefore, the use of such data is encouraged to improve emission quantification methods and advance our understanding of methane cycles.
Antoine Berchet, Isabelle Pison, Camille Huselstein, Clément Narbaud, Marine Remaud, Sauveur Belviso, Camille Abadie, and Fabienne Maignan
Atmos. Chem. Phys., 25, 7499–7525, https://doi.org/10.5194/acp-25-7499-2025, https://doi.org/10.5194/acp-25-7499-2025, 2025
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We use the measurements of atmospheric carbonyl sulfide (COS) concentrations at the monitoring site of Gif-sur-Yvette (in the Paris region) from August 2014 to December 2019, combined with existing knowledge on COS fluxes in the atmosphere and a transport model, to gain insight into COS fluxes, either natural, such as oceanic emissions or vegetation and soil fluxes, or anthropogenic, from industrial activities and power generation.
Jinhui Gao and Hui Xiao
Atmos. Chem. Phys., 25, 7387–7401, https://doi.org/10.5194/acp-25-7387-2025, https://doi.org/10.5194/acp-25-7387-2025, 2025
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The ensemble simulation provides a solution to better reproduce and understand the extremely high ozone episode that occurred in the Great Bay Area when Typhoon Nida approached South China in summer 2016. Elevated temperatures and weak winds contributed to the increase in ozone precursors, resulting in enhanced ozone production. Large amounts of ozone aloft also contributed to the increase in surface ozone via vertical transport. Notably, ozone from Southeast Asia contributed through this mechanism.
Zhenda Sun, Hao Yin, Zhongfeng Pan, Chongyang Li, Xiao Lu, Ke Liu, Youwen Sun, and Cheng Liu
Atmos. Chem. Phys., 25, 6823–6842, https://doi.org/10.5194/acp-25-6823-2025, https://doi.org/10.5194/acp-25-6823-2025, 2025
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This study investigates the variability and driving forces of transboundary CO transport flux over the Tibetan Plateau from May 2018 to April 2024. During this period, external CO influx increased by 2.86 Tg yr-1, while internal efflux slightly declined by 1.70 Tg yr-1. The rising influx in recent years is likely linked to the rapid increase in CO concentrations from South Asia.
Beata Bukosa, Sara Mikaloff-Fletcher, Gordon Brailsford, Dan Smale, Elizabeth D. Keller, W. Troy Baisden, Miko U. F. Kirschbaum, Donna L. Giltrap, Lìyǐn Liáng, Stuart Moore, Rowena Moss, Sylvia Nichol, Jocelyn Turnbull, Alex Geddes, Daemon Kennett, Dóra Hidy, Zoltán Barcza, Louis A. Schipper, Aaron M. Wall, Shin-Ichiro Nakaoka, Hitoshi Mukai, and Andrea Brandon
Atmos. Chem. Phys., 25, 6445–6473, https://doi.org/10.5194/acp-25-6445-2025, https://doi.org/10.5194/acp-25-6445-2025, 2025
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We used atmospheric measurements and inverse modelling to estimate New Zealand's carbon dioxide (CO2) emissions and removals from 2011 to 2020. Our study reveals that New Zealand's land absorbs more CO2 than previously estimated, particularly in areas dominated by indigenous forests. Our results highlight gaps in current national CO2 estimates and methods, suggesting a need for further research to improve emissions reports and refine approaches to track progress toward climate mitigation goals.
Santiago Botía, Saqr Munassar, Thomas Koch, Danilo Custodio, Luana S. Basso, Shujiro Komiya, Jost V. Lavric, David Walter, Manuel Gloor, Giordane Martins, Stijn Naus, Gerbrand Koren, Ingrid T. Luijkx, Stijn Hantson, John B. Miller, Wouter Peters, Christian Rödenbeck, and Christoph Gerbig
Atmos. Chem. Phys., 25, 6219–6255, https://doi.org/10.5194/acp-25-6219-2025, https://doi.org/10.5194/acp-25-6219-2025, 2025
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This study uses dry CO2 mole fractions from the Amazon Tall Tower Observatory together with airborne profiles to estimate net carbon exchange in tropical South America. We found that the biogeographic Amazon is a net carbon sink, while the Cerrado and Caatinga biomes are net carbon sources, resulting in an overall neutral balance. Finally, to further reduce the uncertainty in our estimates we call for an expansion of the monitoring capacity, especially in the Amazon–Andes foothills.
Ioannis Kioutsioukis, Christian Hogrefe, Paul A. Makar, Ummugulsun Alyuz, Jessy O. Bash, Roberto Bellasio, Roberto Bianconi, Tim Buttler, Olivia E. Clifton, Philippe Cheung, Alma Hodzic, Richard Kranenburg, Aurelia Lupascu, Kester Momoh, Juan Luis Perez-Camaño, John Pleim, Young-Hee Ryu, Robero San Jose, Donna Schwede, Ranjeet Sokhi, and Stefano Galmarini
EGUsphere, https://doi.org/10.5194/egusphere-2025-1091, https://doi.org/10.5194/egusphere-2025-1091, 2025
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Deposition is a key in air quality modelling. An evaluation of the AQMEII4 models is performed prior to analysing the different deposition schemes in relation to the LULC used. Such analysis is unprecedented. Among the results, LULC masks have to be harmonised and up-to-date information used in place of outdated and too course masks. Alternatively LULC masks should be evaluated and intercom pared when multiple model results are analysed.
Sepehr Fathi, Paul Makar, Wanmin Gong, Junhua Zhang, Katherine Hayden, and Mark Gordon
Atmos. Chem. Phys., 25, 2385–2405, https://doi.org/10.5194/acp-25-2385-2025, https://doi.org/10.5194/acp-25-2385-2025, 2025
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Our study explores the influence of water phase changes in plumes from industrial sources on atmospheric dispersion of emitted pollutants and air quality. Employing PRISM (Plume-Rise-Iterative-Stratified-Moist), a new method, we found that considering these effects significantly improves predictions of pollutant dispersion. This insight enhances our understanding of environmental impacts, enabling more accurate air quality modelling and fostering more effective pollution management strategies.
Maria K. Tenkanen, Aki Tsuruta, Hugo Denier van der Gon, Lena Höglund-Isaksson, Antti Leppänen, Tiina Markkanen, Ana Maria Roxana Petrescu, Maarit Raivonen, Hermanni Aaltonen, and Tuula Aalto
Atmos. Chem. Phys., 25, 2181–2206, https://doi.org/10.5194/acp-25-2181-2025, https://doi.org/10.5194/acp-25-2181-2025, 2025
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Accurate national methane (CH4) emission estimates are essential for tracking progress towards climate goals. This study compares estimates from Finland, which use different methods and scales, and shows how well a global model estimates emissions within a country. The bottom-up estimates vary a lot, but constraining them with atmospheric CH4 measurements brought the estimates closer together. We also highlight the importance of quantifying natural emissions alongside anthropogenic emissions.
Christian Hogrefe, Stefano Galmarini, Paul A. Makar, Ioannis Kioutsioukis, Olivia E. Clifton, Ummugulsum Alyuz, Jesse O. Bash, Roberto Bellasio, Roberto Bianconi, Tim Butler, Philip Cheung, Alma Hodzic, Richard Kranenburg, Aurelia Lupascu, Kester Momoh, Juan Luis Perez-Camanyo, Jonathan E. Pleim, Young-Hee Ryu, Roberto San Jose, Martijn Schaap, Donna B. Schwede, and Ranjeet Sokhi
EGUsphere, https://doi.org/10.5194/egusphere-2025-225, https://doi.org/10.5194/egusphere-2025-225, 2025
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Performed under the umbrella of the fourth phase of the Air Quality Model Evaluation International Initiative (AQMEII4), this study applies AQMEII4 diagnostic tools to better characterize how dry deposition removes pollutants from the atmosphere in regional-scale models. The results also strongly suggest that improvement and harmonization of the representation of land use in these models would serve the community in their future development efforts.
Xingyu Wang, Fei Jiang, Hengmao Wang, Zhengqi Zhang, Mousong Wu, Jun Wang, Wei He, Weimin Ju, and Jing M. Chen
Atmos. Chem. Phys., 25, 867–880, https://doi.org/10.5194/acp-25-867-2025, https://doi.org/10.5194/acp-25-867-2025, 2025
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The role of OCO-3 XCO2 retrievals in estimating global terrestrial carbon fluxes is unclear. We investigate this by assimilating OCO-3 XCO2 retrievals alone and in combination with OCO-2 XCO2. The assimilation of OCO-3 XCO2 alone underestimates global land sinks, mainly at high latitudes, due to the lack of observations beyond 52° S and 52° N, large variations in the number of data, and varying observation times, while the joint assimilation of OCO-2 and OCO-3 XCO2 has the best performance.
Ke Li, Rong Tan, Wenhao Qiao, Taegyung Lee, Yufen Wang, Danyuting Zhang, Minglong Tang, Wenqing Zhao, Yixuan Gu, Shaojia Fan, Jinqiang Zhang, Xiaopu Lyu, Likun Xue, Jianming Xu, Zhiqiang Ma, Mohd Talib Latif, Teerachai Amnuaylojaroen, Junsu Gil, Mee-Hye Lee, Juseon Bak, Joowan Kim, Hong Liao, Yugo Kanaya, Xiao Lu, Tatsuya Nagashima, and Ja-Ho Koo
EGUsphere, https://doi.org/10.5194/egusphere-2024-3756, https://doi.org/10.5194/egusphere-2024-3756, 2025
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East Asia and Southeast Asia has been identified as a global hot spot with the fastest ozone increase. This paper presents the most comprehensive observational view of ozone distributions and evolution over East Asia and Southeast Asia across different spatiotemporal scales in the past two decades, which will have important implications for assessing ozone impacts on public health and crop yields, and for developing future ozone control strategies.
Zhou Zang, Jane Liu, David Tarasick, Omid Moeini, Jianchun Bian, Jinqiang Zhang, Anne M. Thompson, Roeland Van Malderen, Herman G. J. Smit, Ryan M. Stauffer, Bryan J. Johnson, and Debra E. Kollonige
Atmos. Chem. Phys., 24, 13889–13912, https://doi.org/10.5194/acp-24-13889-2024, https://doi.org/10.5194/acp-24-13889-2024, 2024
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The Trajectory-mapped Ozonesonde dataset for the Stratosphere and Troposphere (TOST) provides a global-scale, long-term ozone climatology that is horizontally and vertically resolved. In this study, we improved, updated and validated TOST from 1970 to 2021. Based on this TOST dataset, we characterized global ozone variations spatially in both the troposphere and stratosphere and temporally by season and decade. We also showed a stagnant lower stratospheric ozone variation since the late 1990s.
Koketso Michelle Molepo, Johannes Bieser, Alkuin Maximilian Koenig, Ian Michael Hedgecock, Ralf Ebinghaus, Aurélien Dommergue, Olivier Magand, Hélène Angot, Oleg Travnikov, Lynwill Martin, Casper Labuschagne, Katie Read, and Yann Bertrand
EGUsphere, https://doi.org/10.5194/egusphere-2024-3722, https://doi.org/10.5194/egusphere-2024-3722, 2024
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Mercury exchange between the ocean and atmosphere is poorly understood due to limited in situ data. Here, using atmospheric mercury observations from ground-based monitoring stations along with air mass trajectories, we found that atmospheric Hg levels increase with air mass ocean exposure time, matching predictions for ocean mercury emissions. This finding indicates that ocean emissions directly influence atmospheric mercury levels and enables us to estimate these emissions on a global scale.
William J. Collins, Fiona M. O'Connor, Connor R. Barker, Rachael E. Byrom, Sebastian D. Eastham, Øivind Hodnebrog, Patrick Jöckel, Eloise A. Marais, Mariano Mertens, Gunnar Myhre, Matthias Nützel, Dirk Olivié, Ragnhild Bieltvedt Skeie, Laura Stecher, Larry W. Horowitz, Vaishali Naik, Gregory Faluvegi, Ulas Im, Lee T. Murray, Drew Shindell, Kostas Tsigaridis, Nathan Luke Abraham, and James Keeble
EGUsphere, https://doi.org/10.5194/egusphere-2024-3698, https://doi.org/10.5194/egusphere-2024-3698, 2024
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If reductions aren’t implemented to limit emissions of pollutants that produce ozone then we calculate that this will cause a warming of climate. We assess how the future warming from ozone is affected by changing meteorological variables such as clouds and atmospheric temperatures. We find that reductions in high cloud cover tend to slightly reduce the warming from ozone.
Kaah P. Menang, Stefan A. Buehler, Lukas Kluft, Robin J. Hogan, and Florian E. Roemer
EGUsphere, https://doi.org/10.5194/egusphere-2024-3051, https://doi.org/10.5194/egusphere-2024-3051, 2024
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We investigated how the uncertainty in representing water vapour continuum absorption in the shortwave affects clear-sky shortwave radiative feedback. For current surface temperature, the impact is modest (<2 %). In a warmer world, continuum induced error in estimated shortwave feedback is up to ~5 %. Using the MT_CKD model in radiative transfer calculations may lead to an underestimation of the shortwave feedback. Constraining shortwave continuum will contribute to reducing these discrepancies.
Kai Meng, Tianliang Zhao, Yongqing Bai, Ming Wu, Le Cao, Xuewei Hou, Yuehan Luo, and Yongcheng Jiang
Atmos. Chem. Phys., 24, 12623–12642, https://doi.org/10.5194/acp-24-12623-2024, https://doi.org/10.5194/acp-24-12623-2024, 2024
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We studied the impact of stratospheric intrusions (SIs) on tropospheric and near-surface ozone in Central and Eastern China from a stratospheric source tracing perspective. SIs contribute the most in the eastern plains, with a contribution exceeding 15 %, and have a small contribution to the west and south. Western Siberia and Mongolia are the most critical source areas for indirect and direct SIs, with the Rossby wave and northeast cold vortex being important driving circulation systems.
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.
Sieglinde Callewaert, Minqiang Zhou, Bavo Langerock, Pucai Wang, Ting Wang, Emmanuel Mahieu, and Martine De Mazière
EGUsphere, https://doi.org/10.5194/egusphere-2024-3228, https://doi.org/10.5194/egusphere-2024-3228, 2024
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We used an atmospheric transport model and satellite data to study CH4 observations at Xianghe, China. Our study shows the key source sectors that influence the concentrations and their respective importance. Furthermore, meteorological factors such as wind direction are discussed. This research highlights the challenges in accurately simulating these kind of measurements and helps us to better understand CH4 variability in the region.
Brian L. Boys, Randall V. Martin, and Trevor C. VandenBoer
EGUsphere, https://doi.org/10.5194/egusphere-2024-2994, https://doi.org/10.5194/egusphere-2024-2994, 2024
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A widely used dry deposition parameterization for NO2 is updated by including a well-known heterogeneous hydrolysis reaction on deposition surfaces. This mechanistic update eliminates a large low bias of -80 % in simulated NO2 nocturnal deposition velocities evaluated against long-term eddy covariance flux observations over Harvard Forest. We highlight the importance of canopy surface area effects as well as soil NO emission in formulating and evaluating NO2 dry deposition parameterizations.
Cynthia D. Nevison, Qing Liang, Paul A. Newman, Britton B. Stephens, Geoff Dutton, Xin Lan, Roisin Commane, Yenny Gonzalez, and Eric Kort
Atmos. Chem. Phys., 24, 10513–10529, https://doi.org/10.5194/acp-24-10513-2024, https://doi.org/10.5194/acp-24-10513-2024, 2024
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This study examines the drivers of interannual variability in tropospheric N2O. New insights are obtained from aircraft data and a chemistry–climate model that explicitly simulates stratospheric N2O. The stratosphere is found to be the dominant driver of N2O variability in the Northern Hemisphere, while both the stratosphere and El Niño cycles are important in the Southern Hemisphere. These results are consistent with known atmospheric dynamics and differences between the hemispheres.
Misa Ishizawa, Douglas Chan, Doug Worthy, Elton Chan, Felix Vogel, Joe R. Melton, and Vivek K. Arora
Atmos. Chem. Phys., 24, 10013–10038, https://doi.org/10.5194/acp-24-10013-2024, https://doi.org/10.5194/acp-24-10013-2024, 2024
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Methane (CH4) emissions in Canada for 2007–2017 were estimated using Canada’s surface greenhouse gas measurements. The estimated emissions show no significant trend, but emission uncertainty was reduced as more measurement sites became available. Notably for climate change, we find the wetland CH4 emissions show a positive correlation with surface air temperature in summer. Canada’s measurement network could monitor future CH4 emission changes and compliance with climate change mitigation goals.
Yiang Chen, Xingcheng Lu, and Jimmy C. H. Fung
Atmos. Chem. Phys., 24, 8847–8864, https://doi.org/10.5194/acp-24-8847-2024, https://doi.org/10.5194/acp-24-8847-2024, 2024
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This study investigates the contribution of pollutants from different emitting periods to ozone episodes over the Greater Bay Area. The analysis reveals the variation in major spatiotemporal contributors to the O3 pollution under the influence of typhoons and subtropical high pressure. Through temporal contribution analysis, our work offers a new perspective on the evolution of O3 pollution and can aid in developing effective and timely control policies under unfavorable weather conditions.
Fabian Maier, Christian Rödenbeck, Ingeborg Levin, Christoph Gerbig, Maksym Gachkivskyi, and Samuel Hammer
Atmos. Chem. Phys., 24, 8183–8203, https://doi.org/10.5194/acp-24-8183-2024, https://doi.org/10.5194/acp-24-8183-2024, 2024
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We investigate the usage of discrete radiocarbon (14C)-based fossil fuel carbon dioxide (ffCO2) concentration estimates vs. continuous carbon monoxide (CO)-based ffCO2 estimates to evaluate the seasonal cycle of ffCO2 emissions in an urban region with an inverse modeling framework. We find that the CO-based ffCO2 estimates allow us to reconstruct robust seasonal cycles, which show the distinct COVID-19 drawdown in 2020 and can be used to validate emission inventories.
Kevin Oliveira, Marc Guevara, Oriol Jorba, Hervé Petetin, Dene Bowdalo, Carles Tena, Gilbert Montané Pinto, Franco López, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 7137–7177, https://doi.org/10.5194/acp-24-7137-2024, https://doi.org/10.5194/acp-24-7137-2024, 2024
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In this work, we assess and evaluate benzene, toluene, and xylene primary emissions and air quality levels in Spain by combining observations, emission inventories, and air quality modelling techniques. The comparison between modelled and observed levels allows identifying uncertainty sources within the emission input. This contributes to improving air quality models' performance when simulating these compounds, leading to better support for the design of effective pollution control strategies.
Yuehan Luo, Tianliang Zhao, Kai Meng, Jun Hu, Qingjian Yang, Yongqing Bai, Kai Yang, Weikang Fu, Chenghao Tan, Yifan Zhang, Yanzhe Zhang, and Zhikuan Li
Atmos. Chem. Phys., 24, 7013–7026, https://doi.org/10.5194/acp-24-7013-2024, https://doi.org/10.5194/acp-24-7013-2024, 2024
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We reveal a significant mechanism of stratospheric O3 intrusion (SI) into the atmospheric environment induced by an extratropical cyclone system. This system facilitates the downward transport of stratospheric O3 to the near-surface layer by vertical coupling, involving the upper westerly trough, the middle northeast cold vortex, and the lower extratropical cyclone in the troposphere. On average, stratospheric O3 contributed 26.77 % to near-surface O3 levels over the North China Plain.
Cheng Zheng, Yutian Wu, Mingfang Ting, and Clara Orbe
Atmos. Chem. Phys., 24, 6965–6985, https://doi.org/10.5194/acp-24-6965-2024, https://doi.org/10.5194/acp-24-6965-2024, 2024
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Trace gases and aerosols in the Arctic, which typically originate from midlatitude and tropical emission regions, modulate the Arctic climate via their radiative and chemistry impacts. Thus, long-range transport of these substances is important for understanding the current and the future change of Arctic climate. By employing chemistry–climate models, we explore how year-to-year variations in the atmospheric circulation modulate atmospheric long-range transport into the Arctic.
Sophie Wittig, Antoine Berchet, Isabelle Pison, Marielle Saunois, and Jean-Daniel Paris
Atmos. Chem. Phys., 24, 6359–6373, https://doi.org/10.5194/acp-24-6359-2024, https://doi.org/10.5194/acp-24-6359-2024, 2024
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The aim of this work is to analyse how accurately a methane bomb event could be detected with the current and a hypothetically extended stationary observation network in the Arctic. For this, we incorporate synthetically modelled possible future CH4 concentrations based on plausible emission scenarios into an inverse modelling framework. We analyse how well the increase is detected in different Arctic regions and evaluate the impact of additional observation sites in this respect.
Vishnu Thilakan, Dhanyalekshmi Pillai, Jithin Sukumaran, Christoph Gerbig, Haseeb Hakkim, Vinayak Sinha, Yukio Terao, Manish Naja, and Monish Vijay Deshpande
Atmos. Chem. Phys., 24, 5315–5335, https://doi.org/10.5194/acp-24-5315-2024, https://doi.org/10.5194/acp-24-5315-2024, 2024
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This study investigates the usability of CO2 mixing ratio observations over India to infer regional carbon sources and sinks. We demonstrate that a high-resolution modelling system can represent the observed CO2 variations reasonably well by improving the transport and flux variations at a fine scale. Future carbon data assimilation systems can thus benefit from these recently available CO2 observations when fine-scale variations are adequately represented in the models.
Rostislav Kouznetsov, Risto Hänninen, Andreas Uppstu, Evgeny Kadantsev, Yalda Fatahi, Marje Prank, Dmitrii Kouznetsov, Steffen Manfred Noe, Heikki Junninen, and Mikhail Sofiev
Atmos. Chem. Phys., 24, 4675–4691, https://doi.org/10.5194/acp-24-4675-2024, https://doi.org/10.5194/acp-24-4675-2024, 2024
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By relying solely on publicly available media reports, we were able to infer the temporal evolution and the injection height for the Nord Stream gas leaks in September 2022. The inventory specifies locations, vertical distributions, and temporal evolution of the methane sources. The inventory can be used to simulate the event with atmospheric transport models. The inventory is supplemented with a set of observational data tailored to evaluate the results of the simulated atmospheric dispersion.
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.
Nan Wang, Hongyue Wang, Xin Huang, Xi Chen, Yu Zou, Tao Deng, Tingyuan Li, Xiaopu Lyu, and Fumo Yang
Atmos. Chem. Phys., 24, 1559–1570, https://doi.org/10.5194/acp-24-1559-2024, https://doi.org/10.5194/acp-24-1559-2024, 2024
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This study explores the influence of extreme-weather-induced natural processes on ozone pollution, which is often overlooked. By analyzing meteorological factors, natural emissions, chemistry pathways and atmospheric transport, we discovered that these natural processes could substantially exacerbate ozone pollution. The findings contribute to a deeper understanding of ozone pollution and offer valuable insights for controlling ozone pollution in the context of global warming.
Jia Mao, Amos P. K. Tai, David H. Y. Yung, Tiangang Yuan, Kong T. Chau, and Zhaozhong Feng
Atmos. Chem. Phys., 24, 345–366, https://doi.org/10.5194/acp-24-345-2024, https://doi.org/10.5194/acp-24-345-2024, 2024
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Surface ozone (O3) is well-known for posing great threats to both human health and agriculture worldwide. However, a multidecadal assessment of the impacts of O3 on public health and agriculture in China is lacking without sufficient O3 observations. We used a hybrid approach combining a chemical transport model and machine learning to provide a robust dataset of O3 concentrations over the past 4 decades in China, thereby filling the gap in the long-term O3 trend and impact assessment in China.
Leon Kuhn, Steffen Beirle, Vinod Kumar, Sergey Osipov, Andrea Pozzer, Tim Bösch, Rajesh Kumar, and Thomas Wagner
Atmos. Chem. Phys., 24, 185–217, https://doi.org/10.5194/acp-24-185-2024, https://doi.org/10.5194/acp-24-185-2024, 2024
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NO₂ is an important air pollutant. It was observed that the WRF-Chem model shows significant deviations in NO₂ abundance when compared to measurements. We use a 1-month simulation over central Europe to show that these deviations can be mostly resolved by reparameterization of the vertical mixing routine. In order to validate our results, they are compared to in situ, satellite, and MAX-DOAS measurements.
Ondřej Tichý, Sabine Eckhardt, Yves Balkanski, Didier Hauglustaine, and Nikolaos Evangeliou
Atmos. Chem. Phys., 23, 15235–15252, https://doi.org/10.5194/acp-23-15235-2023, https://doi.org/10.5194/acp-23-15235-2023, 2023
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We show declining trends in NH3 emissions over Europe for 2013–2020 using advanced dispersion and inverse modelling and satellite measurements from CrIS. Emissions decreased by −26% since 2013, showing that the abatement strategies adopted by the European Union have been very efficient. Ammonia emissions are low in winter and peak in summer due to temperature-dependent soil volatilization. The largest decreases were observed in central and western Europe in countries with high emissions.
Yusuf A. Bhatti, Laura E. Revell, Alex J. Schuddeboom, Adrian J. McDonald, Alex T. Archibald, Jonny Williams, Abhijith U. Venugopal, Catherine Hardacre, and Erik Behrens
Atmos. Chem. Phys., 23, 15181–15196, https://doi.org/10.5194/acp-23-15181-2023, https://doi.org/10.5194/acp-23-15181-2023, 2023
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Aerosols are a large source of uncertainty over the Southern Ocean. A dominant source of sulfate aerosol in this region is dimethyl sulfide (DMS), which is poorly simulated by climate models. We show the sensitivity of simulated atmospheric DMS to the choice of oceanic DMS data set and emission scheme. We show that oceanic DMS has twice the influence on atmospheric DMS than the emission scheme. Simulating DMS more accurately in climate models will help to constrain aerosol uncertainty.
Maryam Golbazi and Cristina Archer
Atmos. Chem. Phys., 23, 15057–15075, https://doi.org/10.5194/acp-23-15057-2023, https://doi.org/10.5194/acp-23-15057-2023, 2023
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We use scientific models to study the impact of ship emissions on air quality along the US East Coast. We find an increase in three major pollutants (PM2.5, NO2, and SO2) in coastal regions. However, we detect a reduction in ozone (O3) levels in major coastal cities. This reduction is linked to the significant emissions of nitrogen oxides (NOx) from ships, which scavenged O3, especially in highly polluted urban areas experiencing an NOx-limited regime.
Xinxu Zhao, Jia Chen, Julia Marshall, Michal Gałkowski, Stephan Hachinger, Florian Dietrich, Ankit Shekhar, Johannes Gensheimer, Adrian Wenzel, and Christoph Gerbig
Atmos. Chem. Phys., 23, 14325–14347, https://doi.org/10.5194/acp-23-14325-2023, https://doi.org/10.5194/acp-23-14325-2023, 2023
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We develop a modeling framework using the Weather Research and Forecasting model at a high spatial resolution (up to 400 m) to simulate atmospheric transport of greenhouse gases and interpret column observations. Output is validated against weather stations and column measurements in August 2018. The differential column method is applied, aided by air-mass transport tracing with the Stochastic Time-Inverted Lagrangian Transport (STILT) model, also for an exploratory measurement interpretation.
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.
Tianfeng Chai, Xinrong Ren, Fong Ngan, Mark Cohen, and Alice Crawford
Atmos. Chem. Phys., 23, 12907–12933, https://doi.org/10.5194/acp-23-12907-2023, https://doi.org/10.5194/acp-23-12907-2023, 2023
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The SO2 emissions of three power plants are estimated using aircraft observations and an ensemble of HYSPLIT dispersion simulations with different plume rise parameters. The emission estimates using the runs with the lowest root mean square errors (RMSEs) and the runs with the best correlation coefficients between the predicted and observed mixing ratios both agree well with the Continuous Emissions Monitoring Systems (CEMS) data. The RMSE-based plume rise appears to be more reasonable.
Jinghui Lian, Thomas Lauvaux, Hervé Utard, François-Marie Bréon, Grégoire Broquet, Michel Ramonet, Olivier Laurent, Ivonne Albarus, Mali Chariot, Simone Kotthaus, Martial Haeffelin, Olivier Sanchez, Olivier Perrussel, Hugo Anne Denier van der Gon, Stijn Nicolaas Camiel Dellaert, and Philippe Ciais
Atmos. Chem. Phys., 23, 8823–8835, https://doi.org/10.5194/acp-23-8823-2023, https://doi.org/10.5194/acp-23-8823-2023, 2023
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This study quantifies urban CO2 emissions via an atmospheric inversion for the Paris metropolitan area over a 6-year period from 2016 to 2021. Results show a long-term decreasing trend of about 2 % ± 0.6 % per year in the annual CO2 emissions over Paris. We conclude that our current capacity can deliver near-real-time CO2 emission estimates at the city scale in under a month, and the results agree within 10 % with independent estimates from multiple city-scale inventories.
Fu-Jie Zhu, Peng-Tuan Hu, and Wan-Li Ma
Atmos. Chem. Phys., 23, 8583–8590, https://doi.org/10.5194/acp-23-8583-2023, https://doi.org/10.5194/acp-23-8583-2023, 2023
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A new steady-state gas–particle partitioning model of polycyclic aromatic hydrocarbons was established based on the level-III multimedia fugacity model, which proved that the particulate proportion of PAHs in emissions was a crucial factor for G–P partitioning of PAHs. In addition, gaseous and particulate interference was also derived in the new steady-state model determined by the particulate proportion in emission that could derivate the G–P partitioning quotients from the equilibrium state.
Christian Hogrefe, Jesse O. Bash, Jonathan E. Pleim, Donna B. Schwede, Robert C. Gilliam, Kristen M. Foley, K. Wyat Appel, and Rohit Mathur
Atmos. Chem. Phys., 23, 8119–8147, https://doi.org/10.5194/acp-23-8119-2023, https://doi.org/10.5194/acp-23-8119-2023, 2023
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Under the umbrella of the fourth phase of the Air Quality Model Evaluation International Initiative (AQMEII4), this study applies AQMEII4 diagnostic tools to better characterize how dry deposition removes pollutants from the atmosphere in the widely used CMAQ model. The results illustrate how these tools can provide insights into similarities and differences between the two CMAQ dry deposition options that affect simulated pollutant budgets and ecosystem impacts from atmospheric pollution.
Kun Qu, Xuesong Wang, Xuhui Cai, Yu Yan, Xipeng Jin, Mihalis Vrekoussis, Maria Kanakidou, Guy P. Brasseur, Jin Shen, Teng Xiao, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 23, 7653–7671, https://doi.org/10.5194/acp-23-7653-2023, https://doi.org/10.5194/acp-23-7653-2023, 2023
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Basic understandings of ozone processes, especially transport and chemistry, are essential to support ozone pollution control, but studies often have different views on their relative importance. We developed a method to quantify their contributions in the ozone mass and concentration budgets based on the WRF-CMAQ model. Results in a polluted region highlight the differences between two budgets. For future studies, two budgets are both needed to fully understand the effects of ozone processes.
Emily Dowd, Chris Wilson, Martyn P. Chipperfield, Emanuel Gloor, Alistair Manning, and Ruth Doherty
Atmos. Chem. Phys., 23, 7363–7382, https://doi.org/10.5194/acp-23-7363-2023, https://doi.org/10.5194/acp-23-7363-2023, 2023
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Surface observations of methane show that the seasonal cycle amplitude (SCA) of methane is decreasing in the northern high latitudes (NHLs) but increased globally (1995–2020). The NHL decrease is counterintuitive, as we expect the SCA to increase with increasing concentrations. We use a chemical transport model to investigate changes in SCA in the NHLs. We find well-mixed methane and changes in emissions from Canada, the Middle East, and Europe are the largest contributors to the SCA in NHLs.
Danyang Ma, Tijian Wang, Hao Wu, Yawei Qu, Jian Liu, Jane Liu, Shu Li, Bingliang Zhuang, Mengmeng Li, and Min Xie
Atmos. Chem. Phys., 23, 6525–6544, https://doi.org/10.5194/acp-23-6525-2023, https://doi.org/10.5194/acp-23-6525-2023, 2023
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Increasing surface ozone (O3) concentrations have long been a significant environmental issue in China, despite the Clean Air Action Plan launched in 2013. Most previous research ignores the contributions of CO2 variations. Our study comprehensively analyzed O3 variation across China from various perspectives and highlighted the importance of considering CO2 variations when designing long-term O3 control policies, especially in high-vegetation-coverage areas.
Jackson Hian-Wui Chang, Stephen M. Griffith, Steven Soon-Kai Kong, Ming-Tung Chuang, and Neng-Huei Lin
Atmos. Chem. Phys., 23, 6357–6382, https://doi.org/10.5194/acp-23-6357-2023, https://doi.org/10.5194/acp-23-6357-2023, 2023
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A novel CMAQ–PMF-based composite index is developed to identify the key VOC source species for an effective ozone abatement strategy. The index provides information as to which VOC species are key to ozone formation and where to reduce sources of these VOC species. Using the composite index, we recommended the VOC control measures in southern Taiwan should prioritize solvent usage, vehicle emissions, and the petrochemical industry.
Lei Duan and Ken Caldeira
Atmos. Chem. Phys., 23, 6011–6020, https://doi.org/10.5194/acp-23-6011-2023, https://doi.org/10.5194/acp-23-6011-2023, 2023
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Ocko and Hamburg (2022) emphasize the short-term climate impact of hydrogen, and we present an analysis that places greater focus on long-term outcomes. We have derived equations that describe the time-evolving impact of hydrogen and show that higher methane leakage is primarily responsible for the warming potential of blue hydrogen, while hydrogen leakage plays a less critical role. Fossil fuels show more prominent longer-term climate impacts than clean hydrogen under all emission scenarios.
Lixu Jin, Wade Permar, Vanessa Selimovic, Damien Ketcherside, Robert J. Yokelson, Rebecca S. Hornbrook, Eric C. Apel, I-Ting Ku, Jeffrey L. Collett Jr., Amy P. Sullivan, Daniel A. Jaffe, Jeffrey R. Pierce, Alan Fried, Matthew M. Coggon, Georgios I. Gkatzelis, Carsten Warneke, Emily V. Fischer, and Lu Hu
Atmos. Chem. Phys., 23, 5969–5991, https://doi.org/10.5194/acp-23-5969-2023, https://doi.org/10.5194/acp-23-5969-2023, 2023
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Short summary
Air quality in the USA has been improving since 1970 due to anthropogenic emission reduction. Those gains have been partly offset by increased wildfire pollution in the western USA in the past 20 years. Still, we do not understand wildfire emissions well due to limited measurements. Here, we used a global transport model to evaluate and constrain current knowledge of wildfire emissions with recent observational constraints, showing the underestimation of wildfire emissions in the western USA.
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a
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Short summary
This paper estimates UK emissions of important greenhouse gases (hydrofluorocarbons (HFCs)) using high-quality atmospheric observations and atmospheric modelling. We compare these estimates with those submitted by the UK to the United Nations. We conclude that global concentrations of these gases are still increasing. Our estimates for the UK are 73 % of those reported and that the UK emissions are now falling, demonstrating an impact of UK government policy.
This paper estimates UK emissions of important greenhouse gases (hydrofluorocarbons (HFCs))...
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