Articles | Volume 22, issue 9
https://doi.org/10.5194/acp-22-6087-2022
© Author(s) 2022. 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-22-6087-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| Highlight paper
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10 May 2022
Research article | Highlight paper |
| 10 May 2022
| 10 May 2022
Projections of hydrofluorocarbon (HFC) emissions and the resulting global warming based on recent trends in observed abundances and current policies
Centre for Environmental Quality, National Institute for Public Health and the Environment (RIVM), P.O. Box 1, 3720 BA Bilthoven, the Netherlands
Institute for Marine and Atmospheric Research Utrecht (IMAU), Utrecht University, Utrecht, the Netherlands
John S. Daniel
NOAA Chemical Sciences Laboratory (CSL), Boulder, Colorado, USA
Stephen A. Montzka
NOAA Global Monitoring Laboratory (GML) Boulder, Colorado, USA
Isaac Vimont
NOAA Global Monitoring Laboratory (GML) Boulder, Colorado, USA
Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA
Matthew Rigby
School of Chemistry, University of Bristol, Bristol, UK
Paul B. Krummel
Climate Science Centre, CSIRO Oceans and Atmosphere, Aspendale, Victoria, Australia
Jens Muhle
Scripps Institution of Oceanography, University of California San Diego, La Jolla, California, USA
Simon O'Doherty
School of Chemistry, University of Bristol, Bristol, UK
Ronald G. Prinn
Center for Global Change Science, Massachusetts Institute of Technology, Cambridge, Massachusetts, USA
Ray F. Weiss
Scripps Institution of Oceanography, University of California San Diego, La Jolla, California, USA
Dickon Young
School of Chemistry, University of Bristol, Bristol, UK
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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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Jin Ma, Linda M. J. Kooijmans, Norbert Glatthor, Stephen A. Montzka, Marc von Hobe, Thomas Röckmann, and Maarten C. Krol
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Hannah Chawner, Karina E. Adcock, Tim Arnold, Yuri Artioli, Caroline Dylag, Grant L. Forster, Anita Ganesan, Heather Graven, Gennadi Lessin, Peter Levy, Ingrid T. Luijx, Alistair Manning, Penelope A. Pickers, Chris Rennick, Christian Rödenbeck, and Matthew Rigby
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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. Discuss., https://doi.org/10.5194/amt-2023-99, https://doi.org/10.5194/amt-2023-99, 2023
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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 Discuss., https://doi.org/10.5194/cp-2023-27, https://doi.org/10.5194/cp-2023-27, 2023
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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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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.
Gabrielle B. Dreyfus, Stephen A. Montzka, Stephen O. Andersen, and Richard Ferris
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2023-53, https://doi.org/10.5194/acp-2023-53, 2023
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The Montreal Protocol has put the ozone layer on a path to recovery by phasing out 99 % of banned ozone-damaging substances. Most of these banned substances are also potent greenhouse gases. Atmospheric monitoring has detected unexpected increases in emissions in several of these banned substances. Here we show how damage to ozone, climate and health can be quantified for these emissions and offset by preventing the equivalent emissions of ozone-damaging substances by destroying existing stocks.
Lei Hu, Deborah Ottinger, Stephanie Bogle, Stephen A. Montzka, Philip L. DeCola, Ed Dlugokencky, Arlyn Andrews, Kirk Thoning, Colm Sweeney, Geoff Dutton, Lauren Aepli, and Andrew Crotwell
Atmos. Chem. Phys., 23, 1437–1448, https://doi.org/10.5194/acp-23-1437-2023, https://doi.org/10.5194/acp-23-1437-2023, 2023
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Effective mitigation of greenhouse gas (GHG) emissions relies on an accurate understanding of emissions. Here we demonstrate the added value of using inventory- and atmosphere-based approaches for estimating US emissions of SF6, the most potent GHG known. The results suggest a large decline in US SF6 emissions, shed light on the possible processes causing the differences between the independent estimates, and identify opportunities for substantial additional emission reductions.
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.
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.
Ranjeet S. Sokhi, Nicolas Moussiopoulos, Alexander Baklanov, John Bartzis, Isabelle Coll, Sandro Finardi, Rainer Friedrich, Camilla Geels, Tiia Grönholm, Tomas Halenka, Matthias Ketzel, Androniki Maragkidou, Volker Matthias, Jana Moldanova, Leonidas Ntziachristos, Klaus Schäfer, Peter Suppan, George Tsegas, Greg Carmichael, Vicente Franco, Steve Hanna, Jukka-Pekka Jalkanen, Guus J. M. Velders, and Jaakko Kukkonen
Atmos. Chem. Phys., 22, 4615–4703, https://doi.org/10.5194/acp-22-4615-2022, https://doi.org/10.5194/acp-22-4615-2022, 2022
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This review of air quality research focuses on developments over the past decade. The article considers current and future challenges that are important from air quality research and policy perspectives and highlights emerging prominent gaps of knowledge. The review also examines how air pollution management needs to adapt to new challenges and makes recommendations to guide the direction for future air quality research within the wider community and to provide support for policy.
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.
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.
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.
Lei Hu, Stephen A. Montzka, Fred Moore, Eric Hintsa, Geoff Dutton, M. Carolina Siso, Kirk Thoning, Robert W. Portmann, Kathryn McKain, Colm Sweeney, Isaac Vimont, David Nance, Bradley Hall, and Steven Wofsy
Atmos. Chem. Phys., 22, 2891–2907, https://doi.org/10.5194/acp-22-2891-2022, https://doi.org/10.5194/acp-22-2891-2022, 2022
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The unexpected increase in CFC-11 emissions between 2012 and 2017 resulted in concerns about delaying the stratospheric ozone recovery. Although the subsequent decline of CFC-11 emissions indicated a mitigation in part to this problem, the regions fully responsible for these large emission changes were unclear. Here, our new estimate, based on atmospheric measurements from two global campaigns and from NOAA, suggests Asia primarily contributed to the global CFC-11 emission rise during 2012–2017.
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.
Andrew Zammit-Mangion, Michael Bertolacci, Jenny Fisher, Ann Stavert, Matthew Rigby, Yi Cao, and Noel Cressie
Geosci. Model Dev., 15, 45–73, https://doi.org/10.5194/gmd-15-45-2022, https://doi.org/10.5194/gmd-15-45-2022, 2022
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We present a framework for estimating the sources and sinks (flux) of carbon dioxide from satellite data. The framework is statistical and yields measures of uncertainty alongside all estimates of flux and other parameters in the underlying model. It also allows us to generate other insights, such as the size of errors and biases in the data. The primary aim of this research was to develop a fully statistical flux inversion framework for use by atmospheric scientists.
Jan C. Minx, William F. Lamb, Robbie M. Andrew, Josep G. Canadell, Monica Crippa, Niklas Döbbeling, Piers M. Forster, Diego Guizzardi, Jos Olivier, Glen P. Peters, Julia Pongratz, Andy Reisinger, Matthew Rigby, Marielle Saunois, Steven J. Smith, Efisio Solazzo, and Hanqin Tian
Earth Syst. Sci. Data, 13, 5213–5252, https://doi.org/10.5194/essd-13-5213-2021, https://doi.org/10.5194/essd-13-5213-2021, 2021
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We provide a synthetic dataset on anthropogenic greenhouse gas (GHG) emissions for 1970–2018 with a fast-track extension to 2019. We show that GHG emissions continued to rise across all gases and sectors. Annual average GHG emissions growth slowed, but absolute decadal increases have never been higher in human history. We identify a number of data gaps and data quality issues in global inventories and highlight their importance for monitoring progress towards international climate goals.
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.
Eric J. Hintsa, Fred L. Moore, Dale F. Hurst, Geoff S. Dutton, Bradley D. Hall, J. David Nance, Ben R. Miller, Stephen A. Montzka, Laura P. Wolton, Audra McClure-Begley, James W. Elkins, Emrys G. Hall, Allen F. Jordan, Andrew W. Rollins, Troy D. Thornberry, Laurel A. Watts, Chelsea R. Thompson, Jeff Peischl, Ilann Bourgeois, Thomas B. Ryerson, Bruce C. Daube, Yenny Gonzalez Ramos, Roisin Commane, Gregory W. Santoni, Jasna V. Pittman, Steven C. Wofsy, Eric Kort, Glenn S. Diskin, and T. Paul Bui
Atmos. Meas. Tech., 14, 6795–6819, https://doi.org/10.5194/amt-14-6795-2021, https://doi.org/10.5194/amt-14-6795-2021, 2021
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We built UCATS to study atmospheric chemistry and transport. It has measured trace gases including CFCs, N2O, SF6, CH4, CO, and H2 with gas chromatography, as well as ozone and water vapor. UCATS has been part of missions to study the tropical tropopause; transport of air into the stratosphere; greenhouse gases, transport, and chemistry in the troposphere; and ozone chemistry, on both piloted and unmanned aircraft. Its design, capabilities, and some results are shown and described here.
Hélène Angot, Connor Davel, Christine Wiedinmyer, Gabrielle Pétron, Jashan Chopra, Jacques Hueber, Brendan Blanchard, Ilann Bourgeois, Isaac Vimont, Stephen A. Montzka, Ben R. Miller, James W. Elkins, and Detlev Helmig
Atmos. Chem. Phys., 21, 15153–15170, https://doi.org/10.5194/acp-21-15153-2021, https://doi.org/10.5194/acp-21-15153-2021, 2021
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After a multidecadal global decline in atmospheric abundance of ethane and propane (precursors of tropospheric ozone and aerosols), previous work showed a reversal of this trend in 2009–2015 in the Northern Hemisphere due to the growth in oil and natural gas production in North America. Here we show a temporary pause in the growth of atmospheric ethane and propane in 2015–2018 and highlight the critical need for additional top-down studies to further constrain ethane and propane emissions.
Liji M. David, Mary Barth, Lena Höglund-Isaksson, Pallav Purohit, Guus J. M. Velders, Sam Glaser, and A. R. Ravishankara
Atmos. Chem. Phys., 21, 14833–14849, https://doi.org/10.5194/acp-21-14833-2021, https://doi.org/10.5194/acp-21-14833-2021, 2021
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We calculated the expected concentrations of trifluoroacetic acid (TFA) from the atmospheric breakdown of HFO-1234yf (CF3CF=CH2), a substitute for global warming hydrofluorocarbons, emitted now and in the future by India, China, and the Middle East. We used two chemical transport models. We conclude that the projected emissions through 2040 would not be detrimental, given the current knowledge of the effects of TFA on humans and ecosystems.
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.
Alistair J. Manning, Alison L. Redington, Daniel Say, Simon O'Doherty, Dickon Young, Peter G. Simmonds, Martin K. Vollmer, Jens Mühle, Jgor Arduini, Gerard Spain, Adam Wisher, Michela Maione, Tanja J. Schuck, Kieran Stanley, Stefan Reimann, Andreas Engel, Paul B. Krummel, Paul J. Fraser, Christina M. Harth, Peter K. Salameh, Ray F. Weiss, Ray Gluckman, Peter N. Brown, John D. Watterson, and Tim Arnold
Atmos. Chem. Phys., 21, 12739–12755, https://doi.org/10.5194/acp-21-12739-2021, https://doi.org/10.5194/acp-21-12739-2021, 2021
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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.
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.
Yenny Gonzalez, Róisín Commane, Ethan Manninen, Bruce C. Daube, Luke D. Schiferl, J. Barry McManus, Kathryn McKain, Eric J. Hintsa, James W. Elkins, Stephen A. Montzka, Colm Sweeney, Fred Moore, Jose L. Jimenez, Pedro Campuzano Jost, Thomas B. Ryerson, Ilann Bourgeois, Jeff Peischl, Chelsea R. Thompson, Eric Ray, Paul O. Wennberg, John Crounse, Michelle Kim, Hannah M. Allen, Paul A. Newman, Britton B. Stephens, Eric C. Apel, Rebecca S. Hornbrook, Benjamin A. Nault, Eric Morgan, and Steven C. Wofsy
Atmos. Chem. Phys., 21, 11113–11132, https://doi.org/10.5194/acp-21-11113-2021, https://doi.org/10.5194/acp-21-11113-2021, 2021
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Vertical profiles of N2O and a variety of chemical species and aerosols were collected nearly from pole to pole over the oceans during the NASA Atmospheric Tomography mission. We observed that tropospheric N2O variability is strongly driven by the influence of stratospheric air depleted in N2O, especially at middle and high latitudes. We also traced the origins of biomass burning and industrial emissions and investigated their impact on the variability of tropospheric N2O.
Fabienne Maignan, Camille Abadie, Marine Remaud, Linda M. J. Kooijmans, Kukka-Maaria Kohonen, Róisín Commane, Richard Wehr, J. Elliott Campbell, Sauveur Belviso, Stephen A. Montzka, Nina Raoult, Ulli Seibt, Yoichi P. Shiga, Nicolas Vuichard, Mary E. Whelan, and Philippe Peylin
Biogeosciences, 18, 2917–2955, https://doi.org/10.5194/bg-18-2917-2021, https://doi.org/10.5194/bg-18-2917-2021, 2021
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The assimilation of carbonyl sulfide (COS) by continental vegetation has been proposed as a proxy for gross primary production (GPP). Using a land surface and a transport model, we compare a mechanistic representation of the plant COS uptake (Berry et al., 2013) to the classical leaf relative uptake (LRU) approach linking GPP and vegetation COS fluxes. We show that at high temporal resolutions a mechanistic approach is mandatory, but at large scales the LRU approach compares similarly.
Stijn Naus, Stephen A. Montzka, Prabir K. Patra, and Maarten C. Krol
Atmos. Chem. Phys., 21, 4809–4824, https://doi.org/10.5194/acp-21-4809-2021, https://doi.org/10.5194/acp-21-4809-2021, 2021
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Following up on previous box model studies, we employ a 3D transport model to estimate variations in the hydroxyl radical (OH) from observations of methyl chloroform (MCF). We derive small interannual OH variations that are consistent with variations in the El Niño–Southern Oscillation. We also find evidence for the release of MCF from oceans in atmospheric gradients of MCF. Both findings highlight the added value of a 3D transport model since box model studies did not identify these effects.
Jin Ma, Linda M. J. Kooijmans, Ara Cho, Stephen A. Montzka, Norbert Glatthor, John R. Worden, Le Kuai, Elliot L. Atlas, and Maarten C. Krol
Atmos. Chem. Phys., 21, 3507–3529, https://doi.org/10.5194/acp-21-3507-2021, https://doi.org/10.5194/acp-21-3507-2021, 2021
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Carbonyl sulfide is an important trace gas in the atmosphere and useful to estimating gross primary productivity in ecosystems, but its sources and sinks remain highly uncertain. Therefore, we applied inverse model system TM5-4DVAR to better constrain the global budget. Our finding is in line with earlier studies, pointing to missing sources in the tropics and more uptake in high latitudes. We also stress the necessity of more ground-based observations and satellite data assimilation in future.
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.
Angharad C. Stell, Luke M. Western, Tomás Sherwen, and Matthew Rigby
Atmos. Chem. Phys., 21, 1717–1736, https://doi.org/10.5194/acp-21-1717-2021, https://doi.org/10.5194/acp-21-1717-2021, 2021
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Although it is the second-most important greenhouse gas, our understanding of the atmospheric-methane budget is limited. The uncertainty highlights the need for new tools to investigate sources and sinks. Here, we use a Gaussian process emulator to efficiently approximate the response of atmospheric-methane observations to changes in the most uncertain emission or loss processes. With this new method, we rigorously quantify the sensitivity of atmospheric observations to budget uncertainties.
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.
Guillaume Monteil, Grégoire Broquet, Marko Scholze, Matthew Lang, Ute Karstens, Christoph Gerbig, Frank-Thomas Koch, Naomi E. Smith, Rona L. Thompson, Ingrid T. Luijkx, Emily White, Antoon Meesters, Philippe Ciais, Anita L. Ganesan, Alistair Manning, Michael Mischurow, Wouter Peters, Philippe Peylin, Jerôme Tarniewicz, Matt Rigby, Christian Rödenbeck, Alex Vermeulen, and Evie M. Walton
Atmos. Chem. Phys., 20, 12063–12091, https://doi.org/10.5194/acp-20-12063-2020, https://doi.org/10.5194/acp-20-12063-2020, 2020
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The paper presents the first results from the EUROCOM project, a regional atmospheric inversion intercomparison exercise involving six European research groups. It aims to produce an estimate of the net carbon flux between the European terrestrial ecosystems and the atmosphere for the period 2006–2015, based on constraints provided by observed CO2 concentrations and using inverse modelling techniques. The use of six different models enables us to investigate the robustness of the results.
Johannes C. Laube, Emma C. Leedham Elvidge, Karina E. Adcock, Bianca Baier, Carl A. M. Brenninkmeijer, Huilin Chen, Elise S. Droste, Jens-Uwe Grooß, Pauli Heikkinen, Andrew J. Hind, Rigel Kivi, Alexander Lojko, Stephen A. Montzka, David E. Oram, Steve Randall, Thomas Röckmann, William T. Sturges, Colm Sweeney, Max Thomas, Elinor Tuffnell, and Felix Ploeger
Atmos. Chem. Phys., 20, 9771–9782, https://doi.org/10.5194/acp-20-9771-2020, https://doi.org/10.5194/acp-20-9771-2020, 2020
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We demonstrate that AirCore technology, which is based on small low-cost balloons, can provide access to trace gas measurements such as CFCs at ultra-low abundances. This is a new way to quantify ozone-depleting, and related, substances in the stratosphere, which is largely inaccessible to aircraft. We show two potential uses: (a) tracking the stratospheric circulation, which is predicted to change, and (b) assessing three common meteorological reanalyses driving a global stratospheric model.
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.
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.
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.
August Andersson, Elena N. Kirillova, Stefano Decesari, Langley DeWitt, Jimmy Gasore, Katherine E. Potter, Ronald G. Prinn, Maheswar Rupakheti, Jean de Dieu Ndikubwimana, Julius Nkusi, and Bonfils Safari
Atmos. Chem. Phys., 20, 4561–4573, https://doi.org/10.5194/acp-20-4561-2020, https://doi.org/10.5194/acp-20-4561-2020, 2020
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Large-scale biomass burning events seasonally cover sub-Saharan Africa with air particles. In this study, we find that the concentrations of these particles at a remote mountain site in Rwanda may increase by a factor of 10 during such dry biomass burning periods, with strong implications for the regional climate and human health. These results provide quantitative constraints that could contribute to reducing the large uncertainties regarding the environmental impact of these fires.
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.
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.
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.
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.
H. Langley DeWitt, Jimmy Gasore, Maheswar Rupakheti, Katherine E. Potter, Ronald G. Prinn, Jean de Dieu Ndikubwimana, Julius Nkusi, and Bonfils Safari
Atmos. Chem. Phys., 19, 2063–2078, https://doi.org/10.5194/acp-19-2063-2019, https://doi.org/10.5194/acp-19-2063-2019, 2019
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Air quality in rapidly developing East Africa is a growing but understudied concern. We analyzed long-term black carbon, carbon monoxide, and ozone measurements from the remote Rwanda Climate Observatory and found that seasonal regional biomass burning raised black carbon levels to above-urban concentrations 6 months out of the year. Additional local pollution could exacerbate this issue. More regional monitoring needs to be done to understand and reduce air pollution in this region.
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.
Stijn Naus, Stephen A. Montzka, Sudhanshu Pandey, Sourish Basu, Ed J. Dlugokencky, and Maarten Krol
Atmos. Chem. Phys., 19, 407–424, https://doi.org/10.5194/acp-19-407-2019, https://doi.org/10.5194/acp-19-407-2019, 2019
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We investigate how the use of a two-box model to describe the troposphere can impact derived results, relative to more complex models. For this, we use a 3-D transport model to tune a two-box model of OH, CH4, and MCF. By comparing the tuned two-box model with a standard model run, we can diagnose and quantify biases inherent to a two-box model. We find strong biases, but these have only a small impact on our final conclusions. However, it is not obvious that this should hold for future studies.
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.
Benjamin Brown-Steiner, Noelle E. Selin, Ronald Prinn, Simone Tilmes, Louisa Emmons, Jean-François Lamarque, and Philip Cameron-Smith
Geosci. Model Dev., 11, 4155–4174, https://doi.org/10.5194/gmd-11-4155-2018, https://doi.org/10.5194/gmd-11-4155-2018, 2018
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We conduct three simulations of atmospheric chemistry using chemical mechanisms of different levels of complexity and compare their results to observations. We explore situations in which the simplified mechanisms match the output of the most complex mechanism, as well as when they diverge. We investigate how concurrent utilization of chemical mechanisms of different complexities can further our atmospheric-chemistry understanding at various scales and give some strategies for future research.
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.
Robyn Butler, Paul I. Palmer, Liang Feng, Stephen J. Andrews, Elliot L. Atlas, Lucy J. Carpenter, Valeria Donets, Neil R. P. Harris, Stephen A. Montzka, Laura L. Pan, Ross J. Salawitch, and Sue M. Schauffler
Atmos. Chem. Phys., 18, 13135–13153, https://doi.org/10.5194/acp-18-13135-2018, https://doi.org/10.5194/acp-18-13135-2018, 2018
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Natural sources of short-lived bromoform and dibromomethane are important for determining the inorganic bromine budget in the stratosphere that drives ozone loss. Two new modelling techniques describe how different geographical source regions influence their atmospheric variability over the western Pacific. We find that it is driven primarily by open ocean sources, and we use atmospheric observations to help estimate their contributions to the upper tropospheric inorganic bromine budget.
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.
Mary E. Whelan, Sinikka T. Lennartz, Teresa E. Gimeno, Richard Wehr, Georg Wohlfahrt, Yuting Wang, Linda M. J. Kooijmans, Timothy W. Hilton, Sauveur Belviso, Philippe Peylin, Róisín Commane, Wu Sun, Huilin Chen, Le Kuai, Ivan Mammarella, Kadmiel Maseyk, Max Berkelhammer, King-Fai Li, Dan Yakir, Andrew Zumkehr, Yoko Katayama, Jérôme Ogée, Felix M. Spielmann, Florian Kitz, Bharat Rastogi, Jürgen Kesselmeier, Julia Marshall, Kukka-Maaria Erkkilä, Lisa Wingate, Laura K. Meredith, Wei He, Rüdiger Bunk, Thomas Launois, Timo Vesala, Johan A. Schmidt, Cédric G. Fichot, Ulli Seibt, Scott Saleska, Eric S. Saltzman, Stephen A. Montzka, Joseph A. Berry, and J. Elliott Campbell
Biogeosciences, 15, 3625–3657, https://doi.org/10.5194/bg-15-3625-2018, https://doi.org/10.5194/bg-15-3625-2018, 2018
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Measurements of the trace gas carbonyl sulfide (OCS) are helpful in quantifying photosynthesis at previously unknowable temporal and spatial scales. While CO2 is both consumed and produced within ecosystems, OCS is mostly produced in the oceans or from specific industries, and destroyed in plant leaves in proportion to CO2. This review summarizes the advancements we have made in the understanding of OCS exchange and applications to vital ecosystem water and carbon cycle questions.
Benjamin Brown-Steiner, Noelle E. Selin, Ronald G. Prinn, Erwan Monier, Simone Tilmes, Louisa Emmons, and Fernando Garcia-Menendez
Atmos. Chem. Phys., 18, 8373–8388, https://doi.org/10.5194/acp-18-8373-2018, https://doi.org/10.5194/acp-18-8373-2018, 2018
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Detecting signals in observations and simulations of atmospheric chemistry is difficult due to the underlying variability in the chemistry, meteorology, and climatology. Here we examine the scale dependence of ozone variability and explore strategies for reducing or averaging this variability and thereby enhancing ozone signal detection capabilities. We find that 10–15 years of temporal averaging, and some level of spatial averaging, reduces the risk of overconfidence in ozone signals.
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.
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 %.
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.
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.
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.
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.
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.
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.
Linda M. J. Kooijmans, Nelly A. M. Uitslag, Mark S. Zahniser, David D. Nelson, Stephen A. Montzka, and Huilin Chen
Atmos. Meas. Tech., 9, 5293–5314, https://doi.org/10.5194/amt-9-5293-2016, https://doi.org/10.5194/amt-9-5293-2016, 2016
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The accuracy of carbon models, used for the prediction of global climate change, is limited by the knowledge of the uptake of carbon by plants through photosynthesis. Carbonyl sulfide (COS) has been suggested as a tracer for this process. To be able to further explore and verify the application of this novel tracer we have tested a laser spectrometer for its suitability to obtain accurate and high precision measurements of COS and CO2 with both laboratory experiments and field measurements.
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.
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.
James H. Butler, Shari A. Yvon-Lewis, Jurgen M. Lobert, Daniel B. King, Stephen A. Montzka, John L. Bullister, Valentin Koropalov, James W. Elkins, Bradley D. Hall, Lei Hu, and Yina Liu
Atmos. Chem. Phys., 16, 10899–10910, https://doi.org/10.5194/acp-16-10899-2016, https://doi.org/10.5194/acp-16-10899-2016, 2016
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This study was conducted to understand the influence of the ocean on the lifetime of atmospheric carbon tetrachloride, a strong, ozone-depleting gas. Data from 16 research cruises conducted between 1987 and 2010 show that, unlike the unreactive chlorofluorocarbons, carbon tetrachloride is undersaturated in surface waters regardless of temperature, wind, or biological regime, but with larger undersaturations with upwelling. Results suggest that the ocean consumes about 18 % of atmospheric CCl4.
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.
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.
Xuekun Fang, Min Shao, Andreas Stohl, Qiang Zhang, Junyu Zheng, Hai Guo, Chen Wang, Ming Wang, Jiamin Ou, Rona L. Thompson, and Ronald G. Prinn
Atmos. Chem. Phys., 16, 3369–3382, https://doi.org/10.5194/acp-16-3369-2016, https://doi.org/10.5194/acp-16-3369-2016, 2016
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This is the first study reporting top-down estimates of benzene and toluene emissions in southern China using atmospheric measurement data from a rural site in the area, an atmospheric transport model and an inverse modeling method. This study shows in detail the temporal and spatial differences between the inversion estimate and four different bottom-up emission inventories (RCP, REAS, MEIC; Yin et al., 2015). We propose that more observations are urgently needed in future.
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.
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.
S. Tegtmeier, F. Ziska, I. Pisso, B. Quack, G. J. M. Velders, X. Yang, and K. Krüger
Atmos. Chem. Phys., 15, 13647–13663, https://doi.org/10.5194/acp-15-13647-2015, https://doi.org/10.5194/acp-15-13647-2015, 2015
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At present, man-made halogens and natural oceanic substances both contribute to the observed ozone depletion. Emissions of the anthropogenic halogens have been reduced, whereas emissions of the natural substances are expected to increase in future climate due to anthropogenic activities affecting oceanic processes. We assess the impact of these oceanic substances on ozone by weighting their emissions with their potential to destroy ozone for current conditions and future projections.
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.
S. T. Lennartz, G. Krysztofiak, C. A. Marandino, B.-M. Sinnhuber, S. Tegtmeier, F. Ziska, R. Hossaini, K. Krüger, S. A. Montzka, E. Atlas, D. E. Oram, T. Keber, H. Bönisch, and B. Quack
Atmos. Chem. Phys., 15, 11753–11772, https://doi.org/10.5194/acp-15-11753-2015, https://doi.org/10.5194/acp-15-11753-2015, 2015
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Marine-produced short-lived trace gases such as halocarbons and DMS significantly impact atmospheric chemistry. To assess this impact on ozone depletion and the radiative budget, it is critical that their marine emissions in atmospheric chemistry models are quantified as accurately as possible. We show that calculating emissions online with an interactive atmosphere improves the agreement with current observations and should be employed regularly in models where marine sources are important.
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.
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. 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.
Emma C. Leedham Elvidge, D. E. Oram, J. C. Laube, A. K. Baker, S. A. Montzka, S. Humphrey, D. A. O'Sullivan, and C. A. M. Brenninkmeijer
Atmos. Chem. Phys., 15, 1939–1958, https://doi.org/10.5194/acp-15-1939-2015, https://doi.org/10.5194/acp-15-1939-2015, 2015
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.
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.
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
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. J. Oltmans, A. Karion, R. C. Schnell, G. Pétron, C. Sweeney, S. Wolter, D. Neff, S. A. Montzka, B. R. Miller, D. Helmig, B. J. Johnson, and J. Hueber
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-14-20117-2014, https://doi.org/10.5194/acpd-14-20117-2014, 2014
Revised manuscript not accepted
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
G. J. M. Velders, S. Solomon, and J. S. Daniel
Atmos. Chem. Phys., 14, 4563–4572, https://doi.org/10.5194/acp-14-4563-2014, https://doi.org/10.5194/acp-14-4563-2014, 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
G. J. M. Velders and J. S. Daniel
Atmos. Chem. Phys., 14, 2757–2776, https://doi.org/10.5194/acp-14-2757-2014, https://doi.org/10.5194/acp-14-2757-2014, 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
L. Kuai, J. Worden, S. S. Kulawik, S. A. Montzka, and J. Liu
Atmos. Meas. Tech., 7, 163–172, https://doi.org/10.5194/amt-7-163-2014, https://doi.org/10.5194/amt-7-163-2014, 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
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
B. W. LaFranchi, G. Pétron, J. B. Miller, S. J. Lehman, A. E. Andrews, E. J. Dlugokencky, B. Hall, B. R. Miller, S. A. Montzka, W. Neff, P. C. Novelli, C. Sweeney, J. C. Turnbull, D. E. Wolfe, P. P. Tans, K. R. Gurney, and T. P. Guilderson
Atmos. Chem. Phys., 13, 11101–11120, https://doi.org/10.5194/acp-13-11101-2013, https://doi.org/10.5194/acp-13-11101-2013, 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
R. Locatelli, P. Bousquet, F. Chevallier, A. Fortems-Cheney, S. Szopa, M. Saunois, A. Agusti-Panareda, D. Bergmann, H. Bian, P. Cameron-Smith, M. P. Chipperfield, E. Gloor, S. Houweling, S. R. Kawa, M. Krol, P. K. Patra, R. G. Prinn, M. Rigby, R. Saito, and C. Wilson
Atmos. Chem. Phys., 13, 9917–9937, https://doi.org/10.5194/acp-13-9917-2013, https://doi.org/10.5194/acp-13-9917-2013, 2013
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
Y. Xu, D. Zaelke, G. J. M. Velders, and V. Ramanathan
Atmos. Chem. Phys., 13, 6083–6089, https://doi.org/10.5194/acp-13-6083-2013, https://doi.org/10.5194/acp-13-6083-2013, 2013
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
B. Hassler, P. J. Young, R. W. Portmann, G. E. Bodeker, J. S. Daniel, K. H. Rosenlof, and S. Solomon
Atmos. Chem. Phys., 13, 5533–5550, https://doi.org/10.5194/acp-13-5533-2013, https://doi.org/10.5194/acp-13-5533-2013, 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. 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
D. A. Belikov, S. Maksyutov, M. Krol, A. Fraser, M. Rigby, H. Bian, A. Agusti-Panareda, D. Bergmann, P. Bousquet, P. Cameron-Smith, M. P. Chipperfield, A. Fortems-Cheiney, E. Gloor, K. Haynes, P. Hess, S. Houweling, S. R. Kawa, R. M. Law, Z. Loh, L. Meng, P. I. Palmer, P. K. Patra, R. G. Prinn, R. Saito, and C. Wilson
Atmos. Chem. Phys., 13, 1093–1114, https://doi.org/10.5194/acp-13-1093-2013, https://doi.org/10.5194/acp-13-1093-2013, 2013
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
The atmospheric oxidizing capacity in China – Part 1: Roles of different photochemical processes
Benefits of net-zero policies for future ozone pollution in China
Simulating impacts on UK air quality from net-zero forest planting scenarios
Understanding offshore high-ozone events during TRACER-AQ 2021 in Houston: insights from WRF–CAMx photochemical modeling
Opinion: Establishing a science-into-policy process for tropospheric ozone assessment
Atmospheric composition and climate impacts of a future hydrogen economy
Assessment of isoprene and near-surface ozone sensitivities to water stress over the Euro-Mediterranean region
Nighttime ozone in the lower boundary layer: insights from 3-year tower-based measurements in South China and regional air quality modeling
What controls ozone sensitivity in the upper tropical troposphere?
Modelling the impacts of emission changes on O3 sensitivity, atmospheric oxidation capacity, and pollution transport over the Catalonia region
A regional modelling study of halogen chemistry within a volcanic plume of Mt Etna's Christmas 2018 eruption
Weekly-derived top-down VOC fluxes over Europe from TROPOMI HCHO data in 2018–2021
Constraining the budget of atmospheric carbonyl sulfide using a 3-D chemical transport model
Atmospheric CO2 inversion reveals the Amazon as a minor carbon source caused by fire emissions, with forest uptake offsetting about half of these emissions
Rapid O3 assimilations – Part 2: Tropospheric O3 changes accompanied by declining NOx emissions in the USA and Europe in 2005–2020
High-resolution air quality simulations of ozone exceedance events during the Lake Michigan Ozone Study
Simulations of winter ozone in the Upper Green River basin, Wyoming, using WRF-Chem
The suitability of atmospheric oxygen measurements to constrain Western European fossil-fuel CO2 emissions and their trends
Measurement report: Assessment of Asian emissions of ethane and propane with a chemistry transport model based on observations from the island of Hateruma
Sensitivity of northeastern US surface ozone predictions to the representation of atmospheric chemistry in the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMMv1.0)
Current status of model predictions on volatile organic compounds and impacts on surface ozone predictions during summer in China
Daytime isoprene nitrates under changing NOx and O3
Atmospheric data support a multi-decadal shift in the global methane budget towards natural tropical emissions
Air quality and related health impact in the UNECE region: source attribution and scenario analysis
Future tropospheric ozone budget and distribution over East Asia under a Net Zero scenario
East Asian methane emissions inferred from high-resolution inversions of GOSAT and TROPOMI observations: a comparative and evaluative analysis
Towards near-real-time air pollutant and greenhouse gas emissions: lessons learned from multiple estimates during the COVID-19 pandemic
Spatiotemporal variation of radionuclide dispersion from nuclear power plant accidents using FLEXPART mini-ensemble modeling
Continuous weekly monitoring of methane emissions from the Permian Basin by inversion of TROPOMI satellite observations
Western European emission estimates of CFC-11, CFC-12 and CCl4 derived from atmospheric measurements from 2008 to 2021
Evaluating modelled tropospheric columns of CH4, CO and O3 in the Arctic using ground-based FTIR measurements
Utility of Geostationary Lightning Mapper Derived Lightning NOx Emission Estimates in Air Quality Modeling Studies
Investigating the differences in calculating global mean surface CO2 abundance: the impact of analysis methodologies and site selection
Estimating methane emissions in the Arctic nations using surface observations from 2008 to 2019
Background nitrogen dioxide (NO2) over the United States and its implications for satellite observations and trends: effects of nitrate photolysis, aircraft, and open fires
Seasonal, interannual and decadal variability of tropospheric ozone in the North Atlantic: comparison of UM-UKCA and remote sensing observations for 2005–2018
Quantification of oil and gas methane emissions in the Delaware and Marcellus basins using a network of continuous tower-based measurements
Insights into Soil NO Emissions and the Contribution to Surface Ozone Formation in China
Global sensitivities of reactive N and S gas and particle concentrations and deposition to precursor emissions reductions
A high-resolution Global Aviation emissions Inventory based on ADS-B (GAIA) for 2019–2021
Large simulated future changes in the nitrate radical under the CMIP6 SSP scenarios: implications for oxidation chemistry
Impact of HO2 aerosol uptake on radical levels and O3 production during summertime in Beijing
Source attribution of near-surface ozone trends in the United States during 1995–2019
Exploring the drivers of tropospheric hydroxyl radical trends in the Geophysical Fluid Dynamics Laboratory AM4.1 atmospheric chemistry–climate model
Comprehensive multiphase chlorine chemistry in the box model CAABA/MECCA: Implications to atmospheric oxidative capacity
Impacts of land cover changes on biogenic emission and its contribution to ozone and secondary organic aerosol in China
High-resolution regional emission inventory contributes to the evaluation of policy effectiveness: a case study in Jiangsu Province, China
Why is ozone in South Korea and the Seoul metropolitan area so high and increasing?
Vehicular ammonia emissions: an underappreciated emission source in densely populated areas
Improving ozone simulations in Asia via multisource data assimilation: results from an observing system simulation experiment with GEMS geostationary satellite observations
Jianing Dai, Guy P. Brasseur, Mihalis Vrekoussis, Maria Kanakidou, Kun Qu, Yijuan Zhang, Hongliang Zhang, and Tao Wang
Atmos. Chem. Phys., 23, 14127–14158, https://doi.org/10.5194/acp-23-14127-2023, https://doi.org/10.5194/acp-23-14127-2023, 2023
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In this study, we used a regional chemical transport model to characterize the different parameters of atmospheric oxidative capacity in recent chemical environments in China. These parameters include the production and destruction rates of ozone and other oxidants, the ozone production efficiency, the OH reactivity, and the length of the reaction chain responsible for the formation of ozone and ROx. They are also affected by the aerosol burden in the atmosphere.
Zhenze Liu, Oliver Wild, Ruth M. Doherty, Fiona M. O'Connor, and Steven T. Turnock
Atmos. Chem. Phys., 23, 13755–13768, https://doi.org/10.5194/acp-23-13755-2023, https://doi.org/10.5194/acp-23-13755-2023, 2023
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We investigate the impact of net-zero policies on surface ozone pollution in China. A chemistry–climate model is used to simulate ozone changes driven by local and external emissions, methane, and warmer climates. A deep learning model is applied to generate more robust ozone projection, and we find that the benefits of net-zero policies may be overestimated with the chemistry–climate model. Nevertheless, it is clear that the policies can still substantially reduce ozone pollution in future.
Gemma Purser, Mathew R. Heal, Edward J. Carnell, Stephen Bathgate, Julia Drewer, James I. L. Morison, and Massimo Vieno
Atmos. Chem. Phys., 23, 13713–13733, https://doi.org/10.5194/acp-23-13713-2023, https://doi.org/10.5194/acp-23-13713-2023, 2023
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Forest expansion is a ″net-zero“ pathway, but change in land cover alters air quality in many ways. This study combines tree planting suitability data with UK measured emissions of biogenic volatile organic compounds to simulate spatial and temporal changes in atmospheric composition for planting scenarios of four species. Decreases in fine particulate matter are relatively larger than increases in ozone, which may indicate a net benefit of tree planting on human health aspects of air quality.
Wei Li, Yuxuan Wang, Xueying Liu, Ehsan Soleimanian, Travis Griggs, James Flynn, and Paul Walter
Atmos. Chem. Phys., 23, 13685–13699, https://doi.org/10.5194/acp-23-13685-2023, https://doi.org/10.5194/acp-23-13685-2023, 2023
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This study examined high offshore ozone events in Galveston Bay and the Gulf of Mexico, using boat data and WRF–CAMx modeling during the TRACER-AQ 2021 field campaign. On average, high ozone is caused by chemistry due to the regional transport of volatile organic compounds and downwind advection of NOx from the ship channel. Two case studies show advection of ozone can be another process leading to high ozone, and accurate wind prediction is crucial for air quality forecasting in coastal areas.
Richard G. Derwent, David D. Parrish, and Ian C. Faloona
Atmos. Chem. Phys., 23, 13613–13623, https://doi.org/10.5194/acp-23-13613-2023, https://doi.org/10.5194/acp-23-13613-2023, 2023
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Elevated tropospheric ozone concentrations driven by anthropogenic precursor emissions are a world-wide health and environmental concern; however, this issue lacks a generally accepted understanding of the scientific issues. Here, we briefly outline the elements required to conduct an international assessment process to establish a conceptual model of the underpinning science and motivate international policy forums for regulating ozone production over hemispheric and global scales.
Nicola J. Warwick, Alex T. Archibald, Paul T. Griffiths, James Keeble, Fiona M. O'Connor, John A. Pyle, and Keith P. Shine
Atmos. Chem. Phys., 23, 13451–13467, https://doi.org/10.5194/acp-23-13451-2023, https://doi.org/10.5194/acp-23-13451-2023, 2023
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A chemistry–climate model has been used to explore the atmospheric response to changes in emissions of hydrogen and other species associated with a shift from fossil fuel to hydrogen use. Leakage of hydrogen results in indirect global warming, offsetting greenhouse gas emission reductions from reduced fossil fuel use. To maximise the benefit of hydrogen as an energy source, hydrogen leakage and emissions of methane, carbon monoxide and nitrogen oxides should be minimised.
Susanna Strada, Andrea Pozzer, Graziano Giuliani, Erika Coppola, Fabien Solmon, Xiaoyan Jiang, Alex Guenther, Efstratios Bourtsoukidis, Dominique Serça, Jonathan Williams, and Filippo Giorgi
Atmos. Chem. Phys., 23, 13301–13327, https://doi.org/10.5194/acp-23-13301-2023, https://doi.org/10.5194/acp-23-13301-2023, 2023
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Water deficit modifies emissions of isoprene, an aromatic compound released by plants that influences the production of an air pollutant such as ozone. Numerical modelling shows that, during the warmest and driest summers, isoprene decreases between −20 and −60 % over the Euro-Mediterranean region, while near-surface ozone only diminishes by a few percent. Decreases in isoprene emissions not only happen under dry conditions, but also could occur after prolonged or repeated water deficits.
Guowen He, Cheng He, Haofan Wang, Xiao Lu, Chenglei Pei, Xiaonuan Qiu, Chenxi Liu, Yiming Wang, Nanxi Liu, Jinpu Zhang, Lei Lei, Yiming Liu, Haichao Wang, Tao Deng, Qi Fan, and Shaojia Fan
Atmos. Chem. Phys., 23, 13107–13124, https://doi.org/10.5194/acp-23-13107-2023, https://doi.org/10.5194/acp-23-13107-2023, 2023
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We analyze nighttime ozone in the lower boundary layer (up to 500 m) from the 2017–2019 measurements at the Canton Tower and the WRF-CMAQ model. We identify a strong ability of the residual layer to store daytime ozone in the convective mixing layer, investigate the chemical and meteorological factors controlling nighttime ozone in the residual layer, and quantify the contribution of nighttime ozone in the residual layer to both the nighttime and the following day’s surface ozone air quality.
Clara M. Nussbaumer, Horst Fischer, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 23, 12651–12669, https://doi.org/10.5194/acp-23-12651-2023, https://doi.org/10.5194/acp-23-12651-2023, 2023
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Ozone is a greenhouse gas and contributes to the earth’s radiative energy budget and therefore to global warming. This effect is the largest in the upper troposphere. In this study, we investigate the processes controlling ozone formation and the sensitivity to its precursors in the upper tropical troposphere based on model simulations by the ECHAM5/MESSy2 Atmospheric Chemistry (EMAC) model. We find that NO𝑥 emissions from lightning most importantly affect ozone chemistry at these altitudes.
Alba Badia, Veronica Vidal, Sergi Ventura, Roger Curcoll, Ricard Segura, and Gara Villalba
Atmos. Chem. Phys., 23, 10751–10774, https://doi.org/10.5194/acp-23-10751-2023, https://doi.org/10.5194/acp-23-10751-2023, 2023
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Improving air quality is a top priority in urban areas. In this study, we used an air quality model to analyse the air quality changes occurring over the metropolitan area of Barcelona and other rural areas affected by transport of the atmospheric plume from the city during mobility restrictions. Our results show that mitigation strategies intended to reduce O3 should be designed according to the local meteorology, air transport, and particular ozone chemistry of the urban area.
Herizo Narivelo, Paul David Hamer, Virginie Marécal, Luke Surl, Tjarda Roberts, Sophie Pelletier, Béatrice Josse, Jonathan Guth, Mickaël Bacles, Simon Warnach, Thomas Wagner, Stefano Corradini, Giuseppe Salerno, and Lorenzo Guerrieri
Atmos. Chem. Phys., 23, 10533–10561, https://doi.org/10.5194/acp-23-10533-2023, https://doi.org/10.5194/acp-23-10533-2023, 2023
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Volcanic emissions emit large quantities of gases and primary aerosols that can play an important role in atmospheric chemistry. We present a study of the fate of volcanic bromine emissions from the eruption of Mount Etna around Christmas 2018. Using a numerical model and satellite observations, we analyse the impact of the volcanic plume and how it modifies the composition of the air over the whole Mediterranean basin, in particular on tropospheric ozone through the bromine-explosion cycle.
Glenn-Michael Oomen, Jean-François Müller, Trissevgeni Stavrakou, Isabelle De Smedt, Thomas Blumenstock, Rigel Kivi, Maria Makarova, Mathias Palm, Amelie Röhling, Yao Té, Corinne Vigouroux, Martina M. Friedrich, Udo Frieß, François Hendrick, Alexis Merlaud, Ankie Piters, Andreas Richter, Michel Van Roozendael, and Thomas Wagner
EGUsphere, https://doi.org/10.5194/egusphere-2023-1972, https://doi.org/10.5194/egusphere-2023-1972, 2023
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Natural emissions from vegetation have a profound impact on air quality for their role in the formation of harmful tropospheric ozone and organic aerosols, yet these emissions are highly uncertain. In this study, we quantify emissions of organic gases over Europe using high-quality satellite measurements of formaldehyde. These satellite observations suggest that emissions from vegetation are much higher than predicted by models, especially in southern Europe.
Michael P. Cartwright, Richard J. Pope, Jeremy J. Harrison, Martyn P. Chipperfield, Chris Wilson, Wuhu Feng, David P. Moore, and Parvadha Suntharalingam
Atmos. Chem. Phys., 23, 10035–10056, https://doi.org/10.5194/acp-23-10035-2023, https://doi.org/10.5194/acp-23-10035-2023, 2023
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A 3-D chemical transport model, TOMCAT, is used to simulate global atmospheric carbonyl sulfide (OCS) distribution. Modelled OCS compares well with satellite observations of OCS from limb-sounding satellite observations. Model simulations also compare adequately with surface and atmospheric observations and suitably capture the seasonality of OCS and background concentrations.
Luana S. Basso, Chris Wilson, Martyn P. Chipperfield, Graciela Tejada, Henrique L. G. Cassol, Egídio Arai, Mathew Williams, T. Luke Smallman, Wouter Peters, Stijn Naus, John B. Miller, and Manuel Gloor
Atmos. Chem. Phys., 23, 9685–9723, https://doi.org/10.5194/acp-23-9685-2023, https://doi.org/10.5194/acp-23-9685-2023, 2023
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The Amazon’s carbon balance may have changed due to forest degradation, deforestation and warmer climate. We used an atmospheric model and atmospheric CO2 observations to quantify Amazonian carbon emissions (2010–2018). The region was a small carbon source to the atmosphere, mostly due to fire emissions. Forest uptake compensated for ~ 50 % of the fire emissions, meaning that the remaining forest is still a small carbon sink. We found no clear evidence of weakening carbon uptake over the period.
Rui Zhu, Zhaojun Tang, Xiaokang Chen, Xiong Liu, and Zhe Jiang
Atmos. Chem. Phys., 23, 9745–9763, https://doi.org/10.5194/acp-23-9745-2023, https://doi.org/10.5194/acp-23-9745-2023, 2023
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Ozone Monitoring Instrument (OMI) and surface O3 observations are used to investigate the changes in tropospheric O3 in the USA and Europe in 2005–2020. The surface-based assimilations show limited changes in surface and tropospheric column O3. The OMI-based assimilations show larger decreases in tropospheric O3 columns in 2010–2014, related to a decline in free-tropospheric NO2. Analysis suggests limited impacts of local emissions decline on tropospheric O3 over the USA and Europe in 2005–2020.
R. Bradley Pierce, Monica Harkey, Allen Lenzen, Lee M. Cronce, Jason A. Otkin, Jonathan L. Case, David S. Henderson, Zac Adelman, Tsengel Nergui, and Christopher R. Hain
Atmos. Chem. Phys., 23, 9613–9635, https://doi.org/10.5194/acp-23-9613-2023, https://doi.org/10.5194/acp-23-9613-2023, 2023
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We evaluate two high-resolution model simulations with different meteorological inputs but identical chemistry and anthropogenic emissions, with the goal of identifying a model configuration best suited for characterizing air quality in locations where lake breezes commonly affect local air quality along the Lake Michigan shoreline. This analysis complements other studies in evaluating the impact of meteorological inputs and parameterizations on air quality in a complex environment.
Shreta Ghimire, Zachary J. Lebo, Shane Murphy, Stefan Rahimi, and Trang Tran
Atmos. Chem. Phys., 23, 9413–9438, https://doi.org/10.5194/acp-23-9413-2023, https://doi.org/10.5194/acp-23-9413-2023, 2023
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High wintertime ozone levels have occurred often in recent years in mountain basins with oil and gas production facilities. Photochemical modeling of ozone production serves as a basis for understanding the mechanism by which it occurs and for predictive capability. We present photochemical model simulations of ozone formation and accumulation in the Upper Green River basin, Wyoming, demonstrating the model's ability to simulate wintertime ozone and the sensitivity of ozone to its precursors.
Christian Rödenbeck, Karina E. Adcock, Markus Eritt, Maksym Gachkivsky, Christoph Gerbig, Samuel Hammer, Armin Jordan, Ralph F. Keeling, Ingeborg Levin, Fabian Maier, Andrew C. Manning, Heiko Moossen, Saqr Munassar, Penelope A. Pickers, Michael Rothe, Yasunori Tohjima, and Sönke Zaehle
EGUsphere, https://doi.org/10.5194/egusphere-2023-767, https://doi.org/10.5194/egusphere-2023-767, 2023
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The carbon dioxide content of the Earth atmosphere is increasing due to human emissions from burning of fossil fuels, causing global climate change. The strength of the fossil-fuel emissions is estimated by inventories based on energy data, but independent validation of these inventories has been recommended by the Intergovernmental Panel on Climate Change. Here we investigate the potential to validate inventories based on measurements of small changes in the atmospheric oxygen content.
Adedayo R. Adedeji, Stephen J. Andrews, Matthew J. Rowlinson, Mathew J. Evans, Alastair C. Lewis, Shigeru Hashimoto, Hitoshi Mukai, Hiroshi Tanimoto, Yasunori Tohjima, and Takuya Saito
Atmos. Chem. Phys., 23, 9229–9244, https://doi.org/10.5194/acp-23-9229-2023, https://doi.org/10.5194/acp-23-9229-2023, 2023
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We use the GEOS-Chem model to interpret observations of CO, C2H6, C3H8, NOx, NOy and O3 made from Hateruma Island in 2018. The model captures many synoptic-scale events and the seasonality of most pollutants at the site but underestimates C2H6 and C3H8 during the winter. These underestimates are unlikely to be reconciled by increases in biomass burning emissions but could be reconciled by increasing the Asian anthropogenic source of C2H6 and C3H8 by factors of around 2 and 3, respectively.
Bryan K. Place, William T. Hutzell, K. Wyat Appel, Sara Farrell, Lukas Valin, Benjamin N. Murphy, Karl M. Seltzer, Golam Sarwar, Christine Allen, Ivan R. Piletic, Emma L. D'Ambro, Emily Saunders, Heather Simon, Ana Torres-Vasquez, Jonathan Pleim, Rebecca H. Schwantes, Matthew M. Coggon, Lu Xu, William R. Stockwell, and Havala O. T. Pye
Atmos. Chem. Phys., 23, 9173–9190, https://doi.org/10.5194/acp-23-9173-2023, https://doi.org/10.5194/acp-23-9173-2023, 2023
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Ground-level ozone is a pollutant with adverse human health and ecosystem effects. Air quality models allow scientists to understand the chemical production of ozone and demonstrate impacts of air quality management plans. In this work, the role of multiple systems in ozone production was investigated for the northeastern US in summer. Model updates to chemical reaction rates and monoterpene chemistry were most influential in decreasing predicted ozone and improving agreement with observations.
Yongliang She, Jingyi Li, Xiaopu Lyu, Hai Guo, Momei Qin, Xiaodong Xie, Kangjia Gong, Fei Ye, Jianjiong Mao, Lin Huang, and Jianlin Hu
EGUsphere, https://doi.org/10.5194/egusphere-2023-1358, https://doi.org/10.5194/egusphere-2023-1358, 2023
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The evaluation of predicted VOC in current chemical transport model is limited in China due to the lack of routine measurements at multiple sites. In this study, we use multi-site VOC measurements to evaluate the CMAQ model predicted VOC and assess the impacts of VOC bias on O3 simulation. Our results demonstrate that current modelling setups and emission inventories are likely to underpredict VOC concentrations, and this underprediction of VOC contributes to lower O3 predictions in China.
Alfred W. Mayhew, Peter M. Edwards, and Jaqueline F. Hamilton
Atmos. Chem. Phys., 23, 8473–8485, https://doi.org/10.5194/acp-23-8473-2023, https://doi.org/10.5194/acp-23-8473-2023, 2023
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Isoprene nitrates are chemical species commonly found in the atmosphere that are important for their impacts on air quality and climate. This paper investigates modelled changes to daytime isoprene nitrate concentrations resulting from changes in NOx and O3. The results highlight the complex, nonlinear chemistry of this group of species under typical conditions for megacities such as Beijing, with many species showing increased concentrations when NOx is decreased and/or ozone is increased.
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.
Claudio A. Belis and Rita Van Dingenen
Atmos. Chem. Phys., 23, 8225–8240, https://doi.org/10.5194/acp-23-8225-2023, https://doi.org/10.5194/acp-23-8225-2023, 2023
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The study assesses the influence that abating emissions in the rest of the world have on exposure and mortality due to ozone and fine particulate matter in the region covered by the Gothenburg protocol (UNECE, mainly Europe and North America). To that end, the impacts of pollutants derived from different geographic areas and anthropogenic sources are analysed in a series of scenarios including measures to abate air pollutants and greenhouse gas emissions with different levels of ambition.
Xuewei Hou, Oliver Wild, Bin Zhu, and James Lee
EGUsphere, https://doi.org/10.5194/egusphere-2023-1592, https://doi.org/10.5194/egusphere-2023-1592, 2023
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In response to the climate crisis, many countries have committed to net zero in a certain future year. The impacts of net zero scenario on tropospheric O3 are less well studied and remain unclear. In this study, we quantified the changes of tropospheric O3 budgets, spatiotemporal distributions of future surface O3 in East Asia and regional O3 source contributions for 2060 under a net zero scenario, using the NCAR Community Earth System Model (CESM) and online O3 tagging methods.
Ruosi Liang, Yuzhong Zhang, Wei Chen, Peixuan Zhang, Jingran Liu, Cuihong Chen, Huiqin Mao, Guofeng Shen, Zhen Qu, Zichong Chen, Minqiang Zhou, Pucai Wang, Robert J. Parker, Hartmut Boesch, Alba Lorente, Joannes D. Maasakkers, and Ilse Aben
Atmos. Chem. Phys., 23, 8039–8057, https://doi.org/10.5194/acp-23-8039-2023, https://doi.org/10.5194/acp-23-8039-2023, 2023
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We compare and evaluate East Asian methane emissions inferred from different satellite observations (GOSAT and TROPOMI). The results show discrepancies over northern India and eastern China. Independent ground-based observations are more consistent with TROPOMI-derived emissions in northern India and GOSAT-derived emissions in eastern China.
Marc Guevara, Hervé Petetin, Oriol Jorba, Hugo Denier van der Gon, Jeroen Kuenen, Ingrid Super, Claire Granier, Thierno Doumbia, Philippe Ciais, Zhu Liu, Robin D. Lamboll, Sabine Schindlbacher, Bradley Matthews, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 23, 8081–8101, https://doi.org/10.5194/acp-23-8081-2023, https://doi.org/10.5194/acp-23-8081-2023, 2023
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This study provides an intercomparison of European 2020 emission changes derived from official inventories, which are reported by countries under the framework of several international conventions and directives, and non-official near-real-time estimates, the use of which has significantly grown since the COVID-19 outbreak. The results of the work are used to produce recommendations on how best to approach and make use of near-real-time emissions for modelling and monitoring applications.
Seyed Omid Nabavi, Theodoros Christoudias, Yiannis Proestos, Christos Fountoukis, Huda Al-Sulaiti, and Jos Lelieveld
Atmos. Chem. Phys., 23, 7719–7739, https://doi.org/10.5194/acp-23-7719-2023, https://doi.org/10.5194/acp-23-7719-2023, 2023
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The objective of our study is to comprehensively assess the timing of radioactive material transportation and deposition, along with the associated population exposure in the designated region. We employed diverse meteorological inputs, emission specifics, and simulation codes, aiming to quantify the level of uncertainty.
Daniel J. Varon, Daniel J. Jacob, Benjamin Hmiel, Ritesh Gautam, David R. Lyon, Mark Omara, Melissa Sulprizio, Lu Shen, Drew Pendergrass, Hannah Nesser, Zhen Qu, Zachary R. Barkley, Natasha L. Miles, Scott J. Richardson, Kenneth J. Davis, Sudhanshu Pandey, Xiao Lu, Alba Lorente, Tobias Borsdorff, Joannes D. Maasakkers, and Ilse Aben
Atmos. Chem. Phys., 23, 7503–7520, https://doi.org/10.5194/acp-23-7503-2023, https://doi.org/10.5194/acp-23-7503-2023, 2023
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We use TROPOMI satellite observations to quantify weekly methane emissions from the US Permian oil and gas basin from May 2018 to October 2020. We find that Permian emissions are highly variable, with diverse economic and activity drivers. The most important drivers during our study period were new well development and natural gas price. Permian methane intensity averaged 4.6 % and decreased by 1 % per year.
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.
Victoria A. Flood, Kimberly Strong, Cynthia H. Whaley, Kaley A. Walker, Thomas Blumenstock, James W. Hannigan, Johan Mellqvist, Justus Notholt, Mathias Palm, Amelie N. Röhling, Stephen Arnold, Stephen Beagley, Rong-You Chien, Jesper Christensen, Makoto Deushi, Srdjan Dobricic, Xinyi Dong, Joshua S. Fu, Michael Gauss, Wanmin Gong, Joakim Langner, Kathy S. Law, Louis Marelle, Tatsuo Onishi, Naga Oshima, David A. Plummer, Luca Pozzoli, Jean-Christophe Raut, Manu A. Thomas, Svetlana Tsyro, and Steven Turnock
EGUsphere, https://doi.org/10.5194/egusphere-2023-1161, https://doi.org/10.5194/egusphere-2023-1161, 2023
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It is important to understand the composition of the Arctic atmosphere and how it is changing. Atmospheric models provide simulations that can inform policy. This study examines simulations of CH4, CO, and O3 by 11 models. Model performance is assessed by comparing results matched in space and time to measurements from five high-latitude ground-based infrared spectrometers. This work finds that models are generally underpredicting the concentrations of these gases in the Arctic troposphere.
Peiyang Cheng, Arastoo Pour-Biazar, Yuling Wu, Shi Kuang, Richard T. McNider, and William J. Koshak
EGUsphere, https://doi.org/10.5194/egusphere-2023-901, https://doi.org/10.5194/egusphere-2023-901, 2023
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Lightning-induced nitrogen monoxide (LNO) emission can be estimated from geostationary satellite observations. The present study uses the LNO emission estimates derived from geostationary satellite observations in an air quality modeling system to investigate the impact of LNO to air quality. Results indicate that significant ozone increase could be due to long-distance chemical transport, lightning activity in the upwind direction, and the mixing of high LNO (or ozone) plumes.
Zhendong Wu, Alex Vermeulen, Yousuke Sawa, Ute Karstens, Wouter Peters, Remco de Kok, Xin Lan, Yasuyuki Nagai, Akinori Ogi, and Oksana Tarasova
EGUsphere, https://doi.org/10.5194/egusphere-2023-1173, https://doi.org/10.5194/egusphere-2023-1173, 2023
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This study focuses on exploring the differences in calculating global surface CO2 and its growth rate, considering the impact of analysis methodologies and site selection. Our study reveals that the current global CO2 network has a good capacity to represent global surface CO2 and its growth rate and trends in atmospheric CO2 mass changes, although small differences exist in different analyses due to the impact of methodology and site selection.
Sophie Wittig, Antoine Berchet, Isabelle Pison, Marielle Saunois, Joël Thanwerdas, Adrien Martinez, Jean-Daniel Paris, Toshinobu Machida, Motoki Sasakawa, Douglas E. J. Worthy, Xin Lan, Rona L. Thompson, Espen Sollum, and Mikhail Arshinov
Atmos. Chem. Phys., 23, 6457–6485, https://doi.org/10.5194/acp-23-6457-2023, https://doi.org/10.5194/acp-23-6457-2023, 2023
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Here, an inverse modelling approach is applied to estimate CH4 sources and sinks in the Arctic from 2008 to 2019. We study the magnitude, seasonal patterns and trends from different sources during recent years. We also assess how the current observation network helps to constrain fluxes. We find that constraints are only significant for North America and, to a lesser extent, West Siberia, where the observation network is relatively dense. We find no clear trend over the period of inversion.
Ruijun Dang, Daniel J. Jacob, Viral Shah, Sebastian D. Eastham, Thibaud M. Fritz, Loretta J. Mickley, Tianjia Liu, Yi Wang, and Jun Wang
Atmos. Chem. Phys., 23, 6271–6284, https://doi.org/10.5194/acp-23-6271-2023, https://doi.org/10.5194/acp-23-6271-2023, 2023
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We use the GEOS-Chem model to better understand the magnitude and trend in free tropospheric NO2 over the contiguous US. Model underestimate of background NO2 is largely corrected by considering aerosol nitrate photolysis. Increase in aircraft emissions affects satellite retrievals by altering the NO2 shape factor, and this effect is expected to increase in future. We show the importance of properly accounting for the free tropospheric background in interpreting NO2 observations from space.
Maria Rosa Russo, Brian John Kerridge, Nathan Luke Abraham, James Keeble, Barry Graham Latter, Richard Siddans, James Weber, Paul Thomas Griffiths, John Adrian Pyle, and Alexander Thomas Archibald
Atmos. Chem. Phys., 23, 6169–6196, https://doi.org/10.5194/acp-23-6169-2023, https://doi.org/10.5194/acp-23-6169-2023, 2023
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Tropospheric ozone is an important component of the Earth system as it can affect both climate and air quality. In this work we use observed tropospheric ozone derived from satellite observations and compare it to tropospheric ozone from model simulations. Our aim is to investigate recent changes (2005–2018) in tropospheric ozone in the North Atlantic region and to understand what factors are driving such changes.
Zachary Barkley, Kenneth Davis, Natasha Miles, Scott Richardson, Aijun Deng, Benjamin Hmiel, David Lyon, and Thomas Lauvaux
Atmos. Chem. Phys., 23, 6127–6144, https://doi.org/10.5194/acp-23-6127-2023, https://doi.org/10.5194/acp-23-6127-2023, 2023
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Using methane monitoring instruments attached to towers, we measure methane concentrations and quantify methane emissions coming from the Marcellus and Permian oil and gas basins. In the Marcellus, emissions were 3 times higher than the state inventory across the entire monitoring period. In the Permian, we see a sharp decline in emissions aligning with the onset of the COVID-19 pandemic. Tower observational networks can be utilized in other basins for long-term monitoring of emissions.
Ling Huang, Jiong Fang, Jiaqiang Liao, Yarwood Greg, Hui Chen, Yangjun Wang, and Li Li
EGUsphere, https://doi.org/10.5194/egusphere-2023-990, https://doi.org/10.5194/egusphere-2023-990, 2023
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Surface ozone concentrations have emerged as a major environmental issue in China. Although control strategies aimed at reducing NOx emissions from conventional combustion sources are widely recognized, soil NOx emissions have received little attention. The impact of soil NO emissions on ground-level ozone concentration is yet to be evaluated. In this study, we estimated the soil NO emissions and evaluated its impact on ozone formation in China.
Yao Ge, Massimo Vieno, David S. Stevenson, Peter Wind, and Mathew R. Heal
Atmos. Chem. Phys., 23, 6083–6112, https://doi.org/10.5194/acp-23-6083-2023, https://doi.org/10.5194/acp-23-6083-2023, 2023
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The sensitivity of fine particles and reactive N and S species to reductions in precursor emissions is investigated using the EMEP MSC-W (European Monitoring and Evaluation Programme Meteorological Synthesizing Centre – West) atmospheric chemistry transport model. This study reveals that the individual emissions reduction has multiple and geographically varying co-benefits and small disbenefits on different species, demonstrating the importance of prioritizing regional emissions controls.
Roger Teoh, Zebediah Engberg, Marc Shapiro, Lynnette Dray, and Marc Stettler
EGUsphere, https://doi.org/10.5194/egusphere-2023-724, https://doi.org/10.5194/egusphere-2023-724, 2023
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Emissions from aircraft contribute to climate change and degrade air quality. We describe an up-to-date 4D emissions inventory of global aviation from 2019 to 2021 based on actual flown trajectories. In 2019, 40.2 million flights collectively travelled 61 billion kilometres using 283 Tg of fuel. Long-haul flights were responsible for 43 % of CO2. The emissions inventory is made available for use in future studies to evaluate the negative externalities arising from global aviation.
Scott Archer-Nicholls, Rachel Allen, Nathan L. Abraham, Paul T. Griffiths, and Alex T. Archibald
Atmos. Chem. Phys., 23, 5801–5813, https://doi.org/10.5194/acp-23-5801-2023, https://doi.org/10.5194/acp-23-5801-2023, 2023
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The nitrate radical is a major oxidant at nighttime, but much less is known about it than about the other oxidants ozone and OH. We use Earth system model calculations to show how the nitrate radical has changed in abundance from 1850–2014 and to 2100 under a range of different climate and emission scenarios. Depending on the emissions and climate scenario, significant increases are projected with implications for the oxidation of volatile organic compounds and the formation of fine aerosol.
Joanna E. Dyson, Lisa K. Whalley, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Stephen D. Worrall, Asan Bacak, Archit Mehra, Thomas J. Bannan, Hugh Coe, Carl J. Percival, Bin Ouyang, C. Nicholas Hewitt, Roderic L. Jones, Leigh R. Crilley, Louisa J. Kramer, W. Joe F. Acton, William J. Bloss, Supattarachai Saksakulkrai, Jingsha Xu, Zongbo Shi, Roy M. Harrison, Simone Kotthaus, Sue Grimmond, Yele Sun, Weiqi Xu, Siyao Yue, Lianfang Wei, Pingqing Fu, Xinming Wang, Stephen R. Arnold, and Dwayne E. Heard
Atmos. Chem. Phys., 23, 5679–5697, https://doi.org/10.5194/acp-23-5679-2023, https://doi.org/10.5194/acp-23-5679-2023, 2023
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The hydroxyl (OH) and closely coupled hydroperoxyl (HO2) radicals are vital for their role in the removal of atmospheric pollutants. In less polluted regions, atmospheric models over-predict HO2 concentrations. In this modelling study, the impact of heterogeneous uptake of HO2 onto aerosol surfaces on radical concentrations and the ozone production regime in Beijing in the summertime is investigated, and the implications for emissions policies across China are considered.
Pengwei Li, Yang Yang, Hailong Wang, Su Li, Ke Li, Pinya Wang, Baojie Li, and Hong Liao
Atmos. Chem. Phys., 23, 5403–5417, https://doi.org/10.5194/acp-23-5403-2023, https://doi.org/10.5194/acp-23-5403-2023, 2023
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We use a novel technique that can attribute O3 to precursors to investigate O3 changes in the United States during 1995–2019. We found that the US domestic energy and surface transportation emission reductions are primarily responsible for the O3 decrease in summer. In winter, factors such as nitrogen oxide emission reduction in the context of its inhibition of ozone production, increased aviation and shipping activities, and large-scale circulation changes contribute to the O3 increases.
Glen Chua, Vaishali Naik, and Larry Wayne Horowitz
Atmos. Chem. Phys., 23, 4955–4975, https://doi.org/10.5194/acp-23-4955-2023, https://doi.org/10.5194/acp-23-4955-2023, 2023
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The hydroxyl radical (OH) is an atmospheric
detergent, removing air pollutants and greenhouse gases like methane from the atmosphere. Thus, understanding how it is changing and responding to its various drivers is important for air quality and climate. We found that OH has increased by about 5 % globally from 1980 to 2014 in our model, mostly driven by increasing nitrogen oxide (NOx) emissions. This suggests potential climate tradeoffs from air quality policies solely targeting NOx emissions.
Meghna Soni, Rolf Sander, Lokesh K. Sahu, Domenico Taraborrelli, Pengfei Liu, Ankit Patel, Imran A. Girach, Andrea Pozzer, Sachin S. Gunthe, and Narendra Ojha
EGUsphere, https://doi.org/10.5194/egusphere-2023-652, https://doi.org/10.5194/egusphere-2023-652, 2023
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The study presents the implementation of comprehensive multiphase chlorine chemistry in the box model CAABA/MECCA. Simulations for contrasting urban environments of Asia and Europe highlight the significant impacts of chlorine on atmospheric oxidation capacity and composition. Chemical processes governing the production and loss of chlorine-containing species have been discussed. The updated chemical mechanism will be useful to interpret field measurements and for future air quality studies.
Jinlong Ma, Shengqiang Zhu, Siyu Wang, Peng Wang, Jianmin Chen, and Hongliang Zhang
Atmos. Chem. Phys., 23, 4311–4325, https://doi.org/10.5194/acp-23-4311-2023, https://doi.org/10.5194/acp-23-4311-2023, 2023
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An updated version of the CMAQ model with biogenic volatile organic compound (BVOC) emissions from MEGAN was applied to study the impacts of different land cover inputs on O3 and secondary organic aerosol (SOA) in China. The estimated BVOC emissions ranged from 25.42 to 37.39 Tg using different leaf area index (LAI) and land cover (LC) inputs. Those differences further induced differences of 4.8–6.9 ppb in O3 concentrations and differences of 5.3–8.4 µg m−3 in SOA concentrations in China.
Chen Gu, Lei Zhang, Zidie Xu, Sijia Xia, Yutong Wang, Li Li, Zeren Wang, Qiuyue Zhao, Hanying Wang, and Yu Zhao
Atmos. Chem. Phys., 23, 4247–4269, https://doi.org/10.5194/acp-23-4247-2023, https://doi.org/10.5194/acp-23-4247-2023, 2023
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We demonstrated the development of a high-resolution emission inventory and its application to evaluate the effectiveness of emission control actions, by incorporating the improved methodology, the best available data, and air quality modeling. We show that substantial efforts for emission controls indeed played an important role in air quality improvement even with worsened meteorological conditions and that the contributions of individual measures to emission reduction were greatly changing.
Nadia K. Colombi, Daniel J. Jacob, Laura Hyesung Yang, Shixian Zhai, Viral Shah, Stuart K. Grange, Robert M. Yantosca, Soontae Kim, and Hong Liao
Atmos. Chem. Phys., 23, 4031–4044, https://doi.org/10.5194/acp-23-4031-2023, https://doi.org/10.5194/acp-23-4031-2023, 2023
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Surface ozone, detrimental to human and ecosystem health, is very high and increasing in South Korea. Using a global model of the atmosphere, we found that emissions from South Korea and China contribute equally to the high ozone observed. We found that in the absence of all anthropogenic emissions over East Asia, ozone is still very high, implying that the air quality standard in South Korea is not practically achievable unless this background external to East Asia can be decreased.
Yifan Wen, Shaojun Zhang, Ye Wu, and Jiming Hao
Atmos. Chem. Phys., 23, 3819–3828, https://doi.org/10.5194/acp-23-3819-2023, https://doi.org/10.5194/acp-23-3819-2023, 2023
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This study established a high-resolution vehicular NH3 emission inventory for mainland China to quantify the absolute value and relative importance of on-road NH3 emissions for different regions, seasons and population densities. Our results indicate that the significant role of on-road NH3 emissions in populated urban areas may have been underappreciated, suggesting the control of vehicular NH3 emission can be a feasible and cost-effective way of mitigating haze pollution in urban areas.
Lei Shu, Lei Zhu, Juseon Bak, Peter Zoogman, Han Han, Song Liu, Xicheng Li, Shuai Sun, Juan Li, Yuyang Chen, Dongchuan Pu, Xiaoxing Zuo, Weitao Fu, Xin Yang, and Tzung-May Fu
Atmos. Chem. Phys., 23, 3731–3748, https://doi.org/10.5194/acp-23-3731-2023, https://doi.org/10.5194/acp-23-3731-2023, 2023
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We quantify the benefit of multisource observations (GEMS, LEO satellite, and surface) on ozone simulations in Asia. Data assimilation improves the monitoring of exceedance, spatial pattern, and diurnal variation of surface ozone, with the regional mean bias reduced from −2.1 to −0.2 ppbv. Data assimilation also better represents ozone vertical distributions in the middle to upper troposphere at low latitudes. Our results offer a valuable reference for future ozone simulations.
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Evidence of a recent decline in UK emissions of hydrofluorocarbons determined by the InTEM inverse model and atmospheric measurements, Atmos. Chem. Phys., 21, 12739–12755, https://doi.org/10.5194/acp-21-12739-2021, 2021.
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Emulating coupled atmosphere-ocean and carbon cycle models with a simpler model, MAGICC6 – Part 1: Model description and calibration, Atmos. Chem. Phys., 11, 1417–1456, https://doi.org/10.5194/acp-11-1417-2011, 2011a.
Meinshausen, M., Wigley, T. M. L., and Raper, S. C. B.:
Emulating atmosphere-ocean and carbon cycle models with a simpler model, MAGICC6 – Part 2: Applications, Atmos. Chem. Phys., 11, 1457–1471, https://doi.org/10.5194/acp-11-1457-2011, 2011b.
METI:
Act on the rational use and proper management of fluorocarbons (Act no. 64 of 2001), http://conf.montreal-protocol.org/meeting/workshops/hfc_management/presentations/Statements by Heads of Delegations/4-Masafumi Ohki_session_4.ppt (last access: 2 October 2015), Ministry of Economy, Trade and Industry, Japan, Tokyo, 2015.
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National greenhouse gas inventory report of Japan, edited by: Studies, N. I. o. E., Center for Global Environmental Research, National Institute for Environmental Studies, National Institute of Environmental Studies, Tsubuka, Japan, 2020.
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History of chemically and radiatively important atmospheric gases from the Advanced Global Atmospheric Gases Experiment (AGAGE), Earth Syst. Sci. Data, 10, 985–1018, https://doi.org/10.5194/essd-10-985-2018, 2018.
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Global emissions of fluorinated greenhouse gases 2005–2050 with abatement potentials and costs, Atmos. Chem. Phys., 17, 2795–2816, https://doi.org/10.5194/acp-17-2795-2017, 2017.
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Electricity savings and greenhouse gas emission reductions from global phase-down of hydrofluorocarbons, Atmos. Chem. Phys., 20, 11305–11327, https://doi.org/10.5194/acp-20-11305-2020, 2020.
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Short summary
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.
The emissions of hydrofluorocarbons (HFCs) have increased significantly in the past as a result...
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