Articles | Volume 16, issue 12
https://doi.org/10.5194/acp-16-7943-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-16-7943-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
30 Jun 2016
Research article |
| 30 Jun 2016
Role of OH variability in the stalling of the global atmospheric CH4 growth rate from 1999 to 2006
School of Earth and Environment, University of Leeds, Leeds, LS2 9JT, UK
National Centre for Earth Observation, University of Leeds, Leeds, LS2 9JT, UK
Martyn P. Chipperfield
School of Earth and Environment, University of Leeds, Leeds, LS2 9JT, UK
National Centre for Earth Observation, University of Leeds, Leeds, LS2 9JT, UK
Manuel Gloor
School of Geography, University of Leeds, Leeds, LS2 9JT, UK
Chris Wilson
School of Earth and Environment, University of Leeds, Leeds, LS2 9JT, UK
National Centre for Earth Observation, University of Leeds, Leeds, LS2 9JT, UK
Wuhu Feng
School of Earth and Environment, University of Leeds, Leeds, LS2 9JT, UK
National Centre for Atmospheric Science, University of Leeds, Leeds, LS2 9JT,
UK
Garry D. Hayman
Centre for Ecology and Hydrology, Wallingford, UK
Matt Rigby
School of Chemistry, University of Bristol, Bristol, BS8 1TS, UK
Paul B. Krummel
CSIRO Oceans and Atmosphere Flagship, Aspendale, Victoria, Australia
Simon O'Doherty
School of Chemistry, University of Bristol, Bristol, BS8 1TS, UK
Ronald G. Prinn
Center for Global Change Science, Massachusetts Instititute of
Technology, Cambridge, MA 02139, USA
Ray F. Weiss
Scripps Institution of Oceanography, University of California, San
Diego, CA 92093, USA
Dickon Young
School of Chemistry, University of Bristol, Bristol, BS8 1TS, UK
Ed Dlugokencky
National Oceanic and Atmospheric Administration, Boulder, CO, USA
Steve A. Montzka
National Oceanic and Atmospheric Administration, Boulder, CO, USA
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Timur Cinay, Dickon Young, Nazaret Narváez Jimenez, Cristina Vintimilla-Palacios, Ariel Pila Alonso, Paul B. Krummel, William Vizuete, and Andrew R. Babbin
EGUsphere, https://doi.org/10.5194/egusphere-2024-3769, https://doi.org/10.5194/egusphere-2024-3769, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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We present the initial 15 months of nitrous oxide measurements from the Galapagos Emissions Monitoring Station. The observed variability in atmospheric mole fractions during this period can be linked to several factors: seasonal variations in trade wind speed and direction across the eastern Pacific, differences in the transport history of air masses sampled, and spatiotemporal heterogeneity in regional marine nitrous oxide emissions from coastal upwelling systems of Peru and Chile.
Matilda A. Pimlott, Richard J. Pope, Brian J. Kerridge, Richard Siddans, Barry G. Latter, Wuhu Feng, and Martyn P. Chipperfield
EGUsphere, https://doi.org/10.5194/egusphere-2024-3717, https://doi.org/10.5194/egusphere-2024-3717, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Tropospheric ozone (O3) is a harmful secondary atmospheric pollutant and an important greenhouse gas. Here, we present an in-depth analysis of lower-tropospheric sub-column O3 (LTCO3, surface – 6 km) records from three satellite products produced by the Rutherford Appleton Laboratory (RAL) over Europe between 1996 and 2017. Overall, we detect moderate negative trends in the satellite records, but corresponding model simulations and ozonesonde measurements show negligible trends.
Ryan Hossaini, David Sherry, Zihao Wang, Martyn P. Chipperfield, Wuhu Feng, David E. Oram, Karina E. Adcock, Stephen A. Montzka, Isobel J. Simpson, Andrea Mazzeo, Amber A. Leeson, Elliot Atlas, and Charles C.-K. Chou
Atmos. Chem. Phys., 24, 13457–13475, https://doi.org/10.5194/acp-24-13457-2024, https://doi.org/10.5194/acp-24-13457-2024, 2024
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DCE (1,2-dichloroethane) is an industrial chemical used to produce PVC (polyvinyl chloride). We analysed DCE production data to estimate global DCE emissions (2002–2020). The emissions were included in an atmospheric model and evaluated by comparing simulated DCE to DCE measurements in the troposphere. We show that DCE contributes ozone-depleting Cl to the stratosphere and that this has increased with increasing DCE emissions. DCE’s impact on stratospheric O3 is currently small but non-zero.
Emma Sands, Richard J. Pope, Ruth M. Doherty, Fiona M. O'Connor, Chris Wilson, and Hugh Pumphrey
Atmos. Chem. Phys., 24, 11081–11102, https://doi.org/10.5194/acp-24-11081-2024, https://doi.org/10.5194/acp-24-11081-2024, 2024
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Changes in vegetation alongside biomass burning impact regional atmospheric composition and air quality. Using satellite remote sensing, we find a clear linear relationship between forest cover and isoprene and a pronounced non-linear relationship between burned area and nitrogen dioxide in the southern Amazon, a region of substantial deforestation. These quantified relationships can be used for model evaluation and further exploration of biosphere-atmosphere interactions in Earth System Models.
Chris Wilson, Brian J. Kerridge, Richard Siddans, David P. Moore, Lucy J. Ventress, Emily Dowd, Wuhu Feng, Martyn P. Chipperfield, and John J. Remedios
Atmos. Chem. Phys., 24, 10639–10653, https://doi.org/10.5194/acp-24-10639-2024, https://doi.org/10.5194/acp-24-10639-2024, 2024
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The leaks from the Nord Stream gas pipelines in September 2022 released a large amount of methane (CH4) into the atmosphere. We provide observational data from a satellite instrument that shows a large CH4 plume over the North Sea off the coast of Scandinavia. We use this together with atmospheric models to quantify the CH4 leaked into the atmosphere from the pipelines. We find that 219–427 Gg CH4 was emitted, making this the largest individual fossil-fuel-related CH4 leak on record.
Matilda A. Pimlott, Richard J. Pope, Brian J. Kerridge, Richard Siddans, Barry G. Latter, Lucy J. Ventress, Wuhu Feng, and Martyn P. Chipperfield
EGUsphere, https://doi.org/10.5194/egusphere-2024-2736, https://doi.org/10.5194/egusphere-2024-2736, 2024
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Globally, lockdowns were implemented to limit the spread of COVID-19, leading to a decrease in emissions of key air pollutants. Here, we use novel satellite data and a chemistry model to investigate the impact of the pandemic on tropospheric ozone (O3), a key pollutant, in 2020. Overall, we found substantial decreases of up to 20 %, 2/3s of which came from emission reductions while 1/3 was due to a decrease in the stratospheric ozone flux into the troposphere.
Alok K. Pandey, David S. Stevenson, Alcide Zhao, Richard J. Pope, Ryan Hossaini, Krishan Kumar, and Marytn P. Chipperfield
EGUsphere, https://doi.org/10.5194/egusphere-2024-2686, https://doi.org/10.5194/egusphere-2024-2686, 2024
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Nitrogen dioxide is an air pollutant largely controlled by human activity that affects ozone, methane and aerosols. Satellite instruments can quantify column NO2, and by carefully matching the time and location of measurements, enable evaluation of model simulations. NO2 over SE Asia is assessed, showing that the model captures many features of the measurements, but also important differences that suggest model deficiencies in representing several aspects of the atmospheric chemistry of NO2.
Gabrielle Pétron, Andrew M. Crotwell, John Mund, Molly Crotwell, Thomas Mefford, Kirk Thoning, Bradley Hall, Duane Kitzis, Monica Madronich, Eric Moglia, Donald Neff, Sonja Wolter, Armin Jordan, Paul Krummel, Ray Langenfelds, and John Patterson
Atmos. Meas. Tech., 17, 4803–4823, https://doi.org/10.5194/amt-17-4803-2024, https://doi.org/10.5194/amt-17-4803-2024, 2024
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Hydrogen (H2) is a gas in trace amounts in the Earth’s atmosphere with indirect impacts on climate and air quality. Renewed interest in H2 as a low- or zero-carbon source of energy may lead to increased production, uses, and supply chain emissions. NOAA measurements of weekly air samples collected between 2009 and 2021 at over 50 sites in mostly remote locations are now available, and they complement other datasets to study the H2 global budget.
Richard J. Pope, Fiona M. O'Connor, Mohit Dalvi, Brian J. Kerridge, Richard Siddans, Barry G. Latter, Brice Barret, Eric Le Flochmoen, Anne Boynard, Martyn P. Chipperfield, Wuhu Feng, Matilda A. Pimlott, Sandip S. Dhomse, Christian Retscher, Catherine Wespes, and Richard Rigby
Atmos. Chem. Phys., 24, 9177–9195, https://doi.org/10.5194/acp-24-9177-2024, https://doi.org/10.5194/acp-24-9177-2024, 2024
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Ozone is a potent air pollutant in the lower troposphere, with adverse impacts on human health. Satellite records of tropospheric ozone currently show large-scale inconsistencies in long-term trends. Our detailed study of the potential factors (e.g. satellite errors, where the satellite can observe ozone) potentially driving these inconsistencies found that, in North America, Europe, and East Asia, the underlying trends are typically small with large uncertainties.
Tahereh Alinejadtabrizi, Yi Huang, Francisco Lang, Steven Siems, Michael Manton, Luis Ackermann, Melita Keywood, Ruhi Humphries, Paul Krummel, Alastair Williams, and Greg Ayers
EGUsphere, https://doi.org/10.5194/egusphere-2024-2397, https://doi.org/10.5194/egusphere-2024-2397, 2024
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Our research explores how weather patterns affect cloud-forming particles (CCN) over the Southern Ocean, crucial for more accurately simulate the Earth's climate. We discovered that winter and summer weather systems significantly influence CCN levels. By analysing air mass trajectories and precipitation, we identified a seasonal cycle in CCN driven by synoptic meteorology. This work enhances climate predictions by improving our understanding of cloud-aerosol interactions in this remote region.
Benjamin Hmiel, Vasilii V. Petrenko, Christo Buizert, Andrew M. Smith, Michael N. Dyonisius, Philip Place, Bin Yang, Quan Hua, Ross Beaudette, Jeffrey P. Severinghaus, Christina Harth, Ray F. Weiss, Lindsey Davidge, Melisa Diaz, Matthew Pacicco, James A. Menking, Michael Kalk, Xavier Faïn, Alden Adolph, Isaac Vimont, and Lee T. Murray
The Cryosphere, 18, 3363–3382, https://doi.org/10.5194/tc-18-3363-2024, https://doi.org/10.5194/tc-18-3363-2024, 2024
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The main aim of this research is to improve understanding of carbon-14 that is produced by cosmic rays in ice sheets. Measurements of carbon-14 in ice cores can provide a range of useful information (age of ice, past atmospheric chemistry, past cosmic ray intensity). Our results show that almost all (>99 %) of carbon-14 that is produced in the upper layer of ice sheets is rapidly lost to the atmosphere. Our results also provide better estimates of carbon-14 production rates in deeper ice.
Yang Li, Wuhu Feng, Xin Zhou, Yajuan Li, and Martyn P. Chipperfield
Atmos. Chem. Phys., 24, 8277–8293, https://doi.org/10.5194/acp-24-8277-2024, https://doi.org/10.5194/acp-24-8277-2024, 2024
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The Tibetan Plateau (TP), the highest and largest plateau, experiences strong surface solar UV radiation, whose excess can cause harmful influences on local biota. Hence, it is critical to study TP ozone. We find ENSO, the strongest interannual phenomenon, tends to induce tropospheric temperature change and thus modulate tropopause variability, which in turn favours ozone change over the TP. Our results have implications for a better understanding of the interannual variability of TP ozone.
Jamal Makkor, Mathias Palm, Matthias Buschmann, Emmanuel Mahieu, Martyn P. Chipperfield, and Justus Notholt
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2024-93, https://doi.org/10.5194/amt-2024-93, 2024
Preprint under review for AMT
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During the years 1950 and 1951, Marcel Migeotte took regular solar measurements in form of paper rolls at the Jungfraujoch site. These historical spectra proved valuable for atmospheric research and needed to be saved for posterity. Therefore, a digitization method which used image processing techniques was developed to extract them from the historical paper rolls. This allowed them to be saved in a machine-readable format that is easily accessible to the scientific community.
Haklim Choi, Alison L. Redington, Hyeri Park, Jooil Kim, Rona L. Thompson, Jens Mühle, Peter K. Salameh, Christina M. Harth, Ray F. Weiss, Alistair J. Manning, and Sunyoung Park
Atmos. Chem. Phys., 24, 7309–7330, https://doi.org/10.5194/acp-24-7309-2024, https://doi.org/10.5194/acp-24-7309-2024, 2024
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We analyzed with an inversion model the atmospheric abundance of hydrofluorocarbons (HFCs), potent greenhouse gases, from 2008 to 2020 at Gosan station in South Korea and revealed a significant increase in emissions, especially from eastern China and Japan. This increase contradicts reported data, underscoring the need for accurate monitoring and reporting. Our findings are crucial for understanding and managing global HFCs emissions, highlighting the importance of efforts to reduce HFCs.
Hanqin Tian, Naiqing Pan, Rona L. Thompson, Josep G. Canadell, Parvadha Suntharalingam, Pierre Regnier, Eric A. Davidson, Michael Prather, Philippe Ciais, Marilena Muntean, Shufen Pan, Wilfried Winiwarter, Sönke Zaehle, Feng Zhou, Robert B. Jackson, Hermann W. Bange, Sarah Berthet, Zihao Bian, Daniele Bianchi, Alexander F. Bouwman, Erik T. Buitenhuis, Geoffrey Dutton, Minpeng Hu, Akihiko Ito, Atul K. Jain, Aurich Jeltsch-Thömmes, Fortunat Joos, Sian Kou-Giesbrecht, Paul B. Krummel, Xin Lan, Angela Landolfi, Ronny Lauerwald, Ya Li, Chaoqun Lu, Taylor Maavara, Manfredi Manizza, Dylan B. Millet, Jens Mühle, Prabir K. Patra, Glen P. Peters, Xiaoyu Qin, Peter Raymond, Laure Resplandy, Judith A. Rosentreter, Hao Shi, Qing Sun, Daniele Tonina, Francesco N. Tubiello, Guido R. van der Werf, Nicolas Vuichard, Junjie Wang, Kelley C. Wells, Luke M. Western, Chris Wilson, Jia Yang, Yuanzhi Yao, Yongfa You, and Qing Zhu
Earth Syst. Sci. Data, 16, 2543–2604, https://doi.org/10.5194/essd-16-2543-2024, https://doi.org/10.5194/essd-16-2543-2024, 2024
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Atmospheric concentrations of nitrous oxide (N2O), a greenhouse gas 273 times more potent than carbon dioxide, have increased by 25 % since the preindustrial period, with the highest observed growth rate in 2020 and 2021. This rapid growth rate has primarily been due to a 40 % increase in anthropogenic emissions since 1980. Observed atmospheric N2O concentrations in recent years have exceeded the worst-case climate scenario, underscoring the importance of reducing anthropogenic N2O emissions.
Dafina Kikaj, Edward Chung, Alan D. Griffiths, Scott D. Chambers, Grant Foster, Angelina Wenger, Penelope Pickers, Chris Rennick, Simon O'Doherty, Joseph Pitt, Kieran Stanley, Dickon Young, Leigh S. Fleming, Karina Adcock, and Tim Arnold
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2024-54, https://doi.org/10.5194/amt-2024-54, 2024
Revised manuscript accepted for AMT
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We present a protocol to enhance confidence in reported atmospheric radon measurements, enabling direct comparisons between sites and integration with GHG measurements. Radon, a natural atmospheric tracer, provides an independent evaluation of transport model performance. The standardized approach ensures radon's use as a metric for model evaluation. Applicable beyond UK observatories, this protocol can benefit larger networks like ICOS or GAW, advancing atmospheric studies worldwide.
Marielle Saunois, Adrien Martinez, Benjamin Poulter, Zhen Zhang, Peter Raymond, Pierre Regnier, Joseph G. Canadell, Robert B. Jackson, Prabir K. Patra, Philippe Bousquet, Philippe Ciais, Edward J. Dlugokencky, Xin Lan, George H. Allen, David Bastviken, David J. Beerling, Dmitry A. Belikov, Donald R. Blake, Simona Castaldi, Monica Crippa, Bridget R. Deemer, Fraser Dennison, Giuseppe Etiope, Nicola Gedney, Lena Höglund-Isaksson, Meredith A. Holgerson, Peter O. Hopcroft, Gustaf Hugelius, Akihito Ito, Atul K. Jain, Rajesh Janardanan, Matthew S. Johnson, Thomas Kleinen, Paul Krummel, Ronny Lauerwald, Tingting Li, Xiangyu Liu, Kyle C. McDonald, Joe R. Melton, Jens Mühle, Jurek Müller, Fabiola Murguia-Flores, Yosuke Niwa, Sergio Noce, Shufen Pan, Robert J. Parker, Changhui Peng, Michel Ramonet, William J. Riley, Gerard Rocher-Ros, Judith A. Rosentreter, Motoki Sasakawa, Arjo Segers, Steven J. Smith, Emily H. Stanley, Joel Thanwerdas, Hanquin Tian, Aki Tsuruta, Francesco N. Tubiello, Thomas S. Weber, Guido van der Werf, Doug E. Worthy, Yi Xi, Yukio Yoshida, Wenxin Zhang, Bo Zheng, Qing Zhu, Qiuan Zhu, and Qianlai Zhuang
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2024-115, https://doi.org/10.5194/essd-2024-115, 2024
Revised manuscript under review for ESSD
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Methane (CH4) is the second most important human-influenced greenhouse gas in terms of climate forcing after carbon dioxide (CO2). A consortium of multi-disciplinary scientists synthesize and update the budget of the sources and sinks of CH4. This edition benefits from important progresses in estimating emissions from lakes and ponds, reservoirs, and streams and rivers. For the 2010s decade, global CH4 emissions are estimated at 575 Tg CH4 yr-1, including ~65 % from anthropogenic sources.
Piers M. Forster, Chris Smith, Tristram Walsh, William F. Lamb, Robin Lamboll, Bradley Hall, Mathias Hauser, Aurélien Ribes, Debbie Rosen, Nathan P. Gillett, Matthew D. Palmer, Joeri Rogelj, Karina von Schuckmann, Blair Trewin, Myles Allen, Robbie Andrew, Richard A. Betts, Alex Borger, Tim Boyer, Jiddu A. Broersma, Carlo Buontempo, Samantha Burgess, Chiara Cagnazzo, Lijing Cheng, Pierre Friedlingstein, Andrew Gettelman, Johannes Gütschow, Masayoshi Ishii, Stuart Jenkins, Xin Lan, Colin Morice, Jens Mühle, Christopher Kadow, John Kennedy, Rachel E. Killick, Paul B. Krummel, Jan C. Minx, Gunnar Myhre, Vaishali Naik, Glen P. Peters, Anna Pirani, Julia Pongratz, Carl-Friedrich Schleussner, Sonia I. Seneviratne, Sophie Szopa, Peter Thorne, Mahesh V. M. Kovilakam, Elisa Majamäki, Jukka-Pekka Jalkanen, Margreet van Marle, Rachel M. Hoesly, Robert Rohde, Dominik Schumacher, Guido van der Werf, Russell Vose, Kirsten Zickfeld, Xuebin Zhang, Valérie Masson-Delmotte, and Panmao Zhai
Earth Syst. Sci. Data, 16, 2625–2658, https://doi.org/10.5194/essd-16-2625-2024, https://doi.org/10.5194/essd-16-2625-2024, 2024
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This paper tracks some key indicators of global warming through time, from 1850 through to the end of 2023. It is designed to give an authoritative estimate of global warming to date and its causes. We find that in 2023, global warming reached 1.3 °C and is increasing at over 0.2 °C per decade. This is caused by all-time-high greenhouse gas emissions.
Jin Ma, Linda M. J. Kooijmans, Norbert Glatthor, Stephen A. Montzka, Marc von Hobe, Thomas Röckmann, and Maarten C. Krol
Atmos. Chem. Phys., 24, 6047–6070, https://doi.org/10.5194/acp-24-6047-2024, https://doi.org/10.5194/acp-24-6047-2024, 2024
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The global budget of atmospheric COS can be optimised by inverse modelling using TM5-4DVAR, with the co-constraints of NOAA surface observations and MIPAS satellite data. We found reduced COS biosphere uptake from inversions and improved land and ocean separation using MIPAS satellite data assimilation. Further improvements are expected from better quantification of COS ocean and biosphere fluxes.
Yiming Xu, Qianlai Zhuang, Bailu Zhao, Michael Billmire, Christopher Cook, Jeremy Graham, Nancy French, and Ronald Prinn
EGUsphere, https://doi.org/10.5194/egusphere-2024-1324, https://doi.org/10.5194/egusphere-2024-1324, 2024
Preprint archived
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We use a process-based model to simulate the fire impacts on soil thermal and hydrological dynamics and carbon budget of forest ecosystems in Northern Eurasia based on satellite-derived burn severity data. We find that fire severity generally increases in this region during the study period. Simulations indicate that fires increase soil temperature and water runoff. Fires lead the forest ecosystems to lose 2.3 Pg C, shifting the forests from a carbon sink to a source in this period.
Felicia Kolonjari, Patrick E. Sheese, Kaley A. Walker, Chris D. Boone, David A. Plummer, Andreas Engel, Stephen A. Montzka, David E. Oram, Tanja Schuck, Gabriele P. Stiller, and Geoffrey C. Toon
Atmos. Meas. Tech., 17, 2429–2449, https://doi.org/10.5194/amt-17-2429-2024, https://doi.org/10.5194/amt-17-2429-2024, 2024
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The Canadian Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS) satellite instrument is currently providing the only vertically resolved chlorodifluoromethane (HCFC-22) measurements from space. This study assesses the most current ACE-FTS HCFC-22 data product in the upper troposphere and lower stratosphere, as well as modelled HCFC-22 from a 39-year run of the Canadian Middle Atmosphere Model (CMAM39) in the same region.
Hannah Chawner, Eric Saboya, Karina E. Adcock, Tim Arnold, Yuri Artioli, Caroline Dylag, Grant L. Forster, Anita Ganesan, Heather Graven, Gennadi Lessin, Peter Levy, Ingrid T. Luijkx, Alistair Manning, Penelope A. Pickers, Chris Rennick, Christian Rödenbeck, and Matthew Rigby
Atmos. Chem. Phys., 24, 4231–4252, https://doi.org/10.5194/acp-24-4231-2024, https://doi.org/10.5194/acp-24-4231-2024, 2024
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The quantity of atmospheric potential oxygen (APO), derived from coincident measurements of carbon dioxide (CO2) and oxygen (O2), has been proposed as a tracer for fossil fuel CO2 emissions. In this model sensitivity study, we examine the use of APO for this purpose in the UK and compare our model to observations. We find that our model simulations are most sensitive to uncertainties relating to ocean fluxes and boundary conditions.
Richard J. Pope, Alexandru Rap, Matilda A. Pimlott, Brice Barret, Eric Le Flochmoen, Brian J. Kerridge, Richard Siddans, Barry G. Latter, Lucy J. Ventress, Anne Boynard, Christian Retscher, Wuhu Feng, Richard Rigby, Sandip S. Dhomse, Catherine Wespes, and Martyn P. Chipperfield
Atmos. Chem. Phys., 24, 3613–3626, https://doi.org/10.5194/acp-24-3613-2024, https://doi.org/10.5194/acp-24-3613-2024, 2024
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Tropospheric ozone is an important short-lived climate forcer which influences the incoming solar short-wave radiation and the outgoing long-wave radiation in the atmosphere (8–15 km) where the balance between the two yields a net positive (i.e. warming) effect at the surface. Overall, we find that the tropospheric ozone radiative effect ranges between 1.21 and 1.26 W m−2 with a negligible trend (2008–2017), suggesting that tropospheric ozone influences on climate have remained stable with time.
Emily Dowd, Alistair J. Manning, Bryn Orth-Lashley, Marianne Girard, James France, Rebecca E. Fisher, Dave Lowry, Mathias Lanoisellé, Joseph R. Pitt, Kieran M. Stanley, Simon O'Doherty, Dickon Young, Glen Thistlethwaite, Martyn P. Chipperfield, Emanuel Gloor, and Chris Wilson
Atmos. Meas. Tech., 17, 1599–1615, https://doi.org/10.5194/amt-17-1599-2024, https://doi.org/10.5194/amt-17-1599-2024, 2024
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We provide the first validation of the satellite-derived emission estimates using surface-based mobile greenhouse gas surveys of an active gas leak detected near Cheltenham, UK. GHGSat’s emission estimates broadly agree with the surface-based mobile survey and steps were taken to fix the leak, highlighting the importance of satellite data in identifying emissions and helping to reduce our human impact on climate change.
Ross Noel Bannister and Chris Wilson
EGUsphere, https://doi.org/10.5194/egusphere-2024-655, https://doi.org/10.5194/egusphere-2024-655, 2024
Preprint archived
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Prior information is essential for the top-down estimation of CH4 surface fluxes. Errors in the prior are correlated in time/space, but accounting for correlations can be costly. We report on an efficient scheme to represent correlations in the inverse modelling system, INVICAT. The method is tested by assimilating CH4 observations using the scheme. Our findings show that accounting for spatio-temporal correlations improve CH4 flux estimates, demonstrating that the method should be further used.
Martyn P. Chipperfield and Slimane Bekki
Atmos. Chem. Phys., 24, 2783–2802, https://doi.org/10.5194/acp-24-2783-2024, https://doi.org/10.5194/acp-24-2783-2024, 2024
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We give a personal perspective on recent issues related to the depletion of stratospheric ozone and some newly emerging challenges. We first provide a brief review of historic work on understanding the ozone layer and review ozone recovery from the effects of halogenated source gases and the Montreal Protocol. We then discuss the recent observations of ozone depletion from Australian fires in early 2020 and the Hunga Tonga–Hunga Ha'apai volcano in January 2022.
Gabrielle B. Dreyfus, Stephen A. Montzka, Stephen O. Andersen, and Richard Ferris
Atmos. Chem. Phys., 24, 2023–2032, https://doi.org/10.5194/acp-24-2023-2024, https://doi.org/10.5194/acp-24-2023-2024, 2024
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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 substances are also potent greenhouse gases. Atmospheric monitoring has detected unexpected increases in emissions in several of these banned substances. Here we present an approach for quantifying damage to ozone, climate and health for these emissions and offset by preventing the equivalent emissions of ozone-damaging substances.
Rona L. Thompson, Stephen A. Montzka, Martin K. Vollmer, Jgor Arduini, Molly Crotwell, Paul B. Krummel, Chris Lunder, Jens Mühle, Simon O'Doherty, Ronald G. Prinn, Stefan Reimann, Isaac Vimont, Hsiang Wang, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 24, 1415–1427, https://doi.org/10.5194/acp-24-1415-2024, https://doi.org/10.5194/acp-24-1415-2024, 2024
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The hydroxyl radical determines the atmospheric lifetimes of numerous species including methane. Since OH is very short-lived, it is not possible to directly measure its concentration on scales relevant for understanding its effect on other species. Here, OH is inferred by looking at changes in hydrofluorocarbons (HFCs). We find that OH levels have been fairly stable over our study period (2004 to 2021), suggesting that OH is not the main driver of the recent increase in atmospheric methane.
Ailish M. Graham, Richard J. Pope, Martyn P. Chipperfield, Sandip S. Dhomse, Matilda Pimlott, Wuhu Feng, Vikas Singh, Ying Chen, Oliver Wild, Ranjeet Sokhi, and Gufran Beig
Atmos. Chem. Phys., 24, 789–806, https://doi.org/10.5194/acp-24-789-2024, https://doi.org/10.5194/acp-24-789-2024, 2024
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Our paper uses novel satellite datasets and high-resolution emissions datasets alongside a back-trajectory model to investigate the balance of local and external sources influencing NOx air pollution changes in Delhi. We find in the post-monsoon season that NOx from local and non-local transport emissions contributes most to poor air quality in Delhi. Therefore, air quality mitigation strategies in Delhi and surrounding regions are used to control this issue.
Tanja J. Schuck, Johannes Degen, Eric Hintsa, Peter Hoor, Markus Jesswein, Timo Keber, Daniel Kunkel, Fred Moore, Florian Obersteiner, Matt Rigby, Thomas Wagenhäuser, Luke M. Western, Andreas Zahn, and Andreas Engel
Atmos. Chem. Phys., 24, 689–705, https://doi.org/10.5194/acp-24-689-2024, https://doi.org/10.5194/acp-24-689-2024, 2024
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We study the interhemispheric gradient of sulfur hexafluoride (SF6), a strong long-lived greenhouse gas. Its emissions are stronger in the Northern Hemisphere; therefore, mixing ratios in the Southern Hemisphere lag behind. Comparing the observations to a box model, the model predicts air in the Southern Hemisphere to be older. For a better agreement, the emissions used as model input need to be increased (and their spatial pattern changed), and we need to modify north–south transport.
Andrea Pazmiño, Florence Goutail, Sophie Godin-Beekmann, Alain Hauchecorne, Jean-Pierre Pommereau, Martyn P. Chipperfield, Wuhu Feng, Franck Lefèvre, Audrey Lecouffe, Michel Van Roozendael, Nis Jepsen, Georg Hansen, Rigel Kivi, Kimberly Strong, and Kaley A. Walker
Atmos. Chem. Phys., 23, 15655–15670, https://doi.org/10.5194/acp-23-15655-2023, https://doi.org/10.5194/acp-23-15655-2023, 2023
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The vortex-averaged ozone loss over the last 3 decades is evaluated for both polar regions using the passive ozone tracer of the chemical transport model TOMCAT/SLIMCAT and total ozone observations from the SAOZ network and MSR2 reanalysis. Three metrics were developed to compute ozone trends since 2000. The study confirms the ozone recovery in the Antarctic and shows a potential sign of quantitative detection of ozone recovery in the Arctic that needs to be robustly confirmed in the future.
Douglas E. J. Worthy, Michele K. Rauh, Lin Huang, Felix R. Vogel, Alina Chivulescu, Kenneth A. Masarie, Ray L. Langenfelds, Paul B. Krummel, Colin E. Allison, Andrew M. Crotwell, Monica Madronich, Gabrielle Pétron, Ingeborg Levin, Samuel Hammer, Sylvia Michel, Michel Ramonet, Martina Schmidt, Armin Jordan, Heiko Moossen, Michael Rothe, Ralph Keeling, and Eric J. Morgan
Atmos. Meas. Tech., 16, 5909–5935, https://doi.org/10.5194/amt-16-5909-2023, https://doi.org/10.5194/amt-16-5909-2023, 2023
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Network compatibility is important for inferring greenhouse gas fluxes at global or regional scales. This study is the first assessment of the measurement agreement among seven individual programs within the World Meteorological Organization community. It compares co-located flask air measurements at the Alert Observatory in Canada over a 17-year period. The results provide stronger confidence in the uncertainty estimation while using those datasets in various data interpretation applications.
John D. Patterson, Murat Aydin, Andrew M. Crotwell, Gabrielle Pétron, Jeffery P. Severinghaus, Paul B. Krummel, Ray L. Langenfelds, Vasilii V. Petrenko, and Eric S. Saltzman
Clim. Past, 19, 2535–2550, https://doi.org/10.5194/cp-19-2535-2023, https://doi.org/10.5194/cp-19-2535-2023, 2023
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Atmospheric levels of molecular hydrogen (H2) can impact climate and air quality. Constraining past changes to atmospheric H2 is useful for understanding how H2 cycles through the Earth system and predicting the impacts of increasing anthropogenic emissions under the
hydrogen economy. Here, we use the aging air found in the polar snowpack to reconstruct H2 levels over the past 100 years. We find that H2 levels increased by 30 % over Greenland and 60 % over Antarctica during the 20th century.
Richard J. Pope, Brian J. Kerridge, Richard Siddans, Barry G. Latter, Martyn P. Chipperfield, Wuhu Feng, Matilda A. Pimlott, Sandip S. Dhomse, Christian Retscher, and Richard Rigby
Atmos. Chem. Phys., 23, 14933–14947, https://doi.org/10.5194/acp-23-14933-2023, https://doi.org/10.5194/acp-23-14933-2023, 2023
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Ozone is a potent air pollutant, and we present the first study to investigate long-term changes in lower tropospheric column ozone (LTCO3) from space. We have constructed a merged LTCO3 dataset from GOME-1, SCIAMACHY and OMI between 1996 and 2017. Comparing LTCO3 between the 1996–2000 and 2013–2017 5-year averages, we find significant positive increases in the tropics/sub-tropics, while in the northern mid-latitudes, we find small-scale differences.
Sandip S. Dhomse and Martyn P. Chipperfield
Earth Syst. Sci. Data, 15, 5105–5120, https://doi.org/10.5194/essd-15-5105-2023, https://doi.org/10.5194/essd-15-5105-2023, 2023
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There are no long-term stratospheric profile data sets for two very important greenhouse gases: methane (CH4) and nitrous oxide (N2O). Along with radiative feedback, these species play an important role in controlling ozone loss in the stratosphere. Here, we use machine learning to fuse satellite measurements with a chemical model to construct long-term gap-free profile data sets for CH4 and N2O. We aim to construct similar data sets for other important trace gases (e.g. O3, Cly, NOy species).
Ioannis Katharopoulos, Dominique Rust, Martin K. Vollmer, Dominik Brunner, Stefan Reimann, Simon J. O'Doherty, Dickon Young, Kieran M. Stanley, Tanja Schuck, Jgor Arduini, Lukas Emmenegger, and Stephan Henne
Atmos. Chem. Phys., 23, 14159–14186, https://doi.org/10.5194/acp-23-14159-2023, https://doi.org/10.5194/acp-23-14159-2023, 2023
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The effectiveness of climate change mitigation needs to be scrutinized by monitoring greenhouse gas (GHG) emissions. Countries report their emissions to the UN in a bottom-up manner. By combining atmospheric observations and transport models someone can independently validate emission estimates in a top-down fashion. We report Swiss emissions of synthetic GHGs based on kilometer-scale transport and inverse modeling, highlighting the role of appropriate resolution in complex terrain.
Ewa M. Bednarz, Ryan Hossaini, and Martyn P. Chipperfield
Atmos. Chem. Phys., 23, 13701–13711, https://doi.org/10.5194/acp-23-13701-2023, https://doi.org/10.5194/acp-23-13701-2023, 2023
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We quantify, for the first time, the time-varying impact of uncontrolled emissions of chlorinated very short-lived substances (Cl-VSLSs) on stratospheric ozone using a state-of-the-art chemistry-climate model. We demonstrate that Cl-VSLSs already have a non-negligible impact on stratospheric ozone, including a local reduction of up to ~7 DU in Arctic ozone in the cold winter of 2019/20, and any so future growth in emissions will continue to offset some of the benefits of the Montreal Protocol.
Ewa M. Bednarz, Ryan Hossaini, N. Luke Abraham, and Martyn P. Chipperfield
Geosci. Model Dev., 16, 6187–6209, https://doi.org/10.5194/gmd-16-6187-2023, https://doi.org/10.5194/gmd-16-6187-2023, 2023
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Development and performance of the new DEST chemistry scheme of UM–UKCA is described. The scheme extends the standard StratTrop scheme by including important updates to the halogen chemistry, thus allowing process-oriented studies of stratospheric ozone depletion and recovery, including impacts from both controlled long-lived ozone-depleting substances and emerging issues around uncontrolled, very short-lived substances. It will thus aid studies in support of future ozone assessment reports.
Richard J. Pope, Brian J. Kerridge, Martyn P. Chipperfield, Richard Siddans, Barry G. Latter, Lucy J. Ventress, Matilda A. Pimlott, Wuhu Feng, Edward Comyn-Platt, Garry D. Hayman, Stephen R. Arnold, and Ailish M. Graham
Atmos. Chem. Phys., 23, 13235–13253, https://doi.org/10.5194/acp-23-13235-2023, https://doi.org/10.5194/acp-23-13235-2023, 2023
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In the summer of 2018, Europe experienced several persistent large-scale ozone (O3) pollution episodes. Satellite tropospheric O3 and surface O3 data recorded substantial enhancements in 2018 relative to other years. Targeted model simulations showed that meteorological processes and emissions controlled the elevated surface O3, while mid-tropospheric O3 enhancements were dominated by stratospheric O3 intrusion and advection of North Atlantic O3-rich air masses into Europe.
Yajuan Li, Sandip S. Dhomse, Martyn P. Chipperfield, Wuhu Feng, Jianchun Bian, Yuan Xia, and Dong Guo
Atmos. Chem. Phys., 23, 13029–13047, https://doi.org/10.5194/acp-23-13029-2023, https://doi.org/10.5194/acp-23-13029-2023, 2023
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For the first time a regularized multivariate regression model is used to estimate stratospheric ozone trends. Regularized regression avoids the over-fitting issue due to correlation among explanatory variables. We demonstrate that there are considerable differences in satellite-based and chemical-model-based ozone trends, highlighting large uncertainties in our understanding about ozone variability. We argue that caution is needed when interpreting results with different methods and datasets.
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.
Hyeri Park, Jooil Kim, Haklim Choi, Sohyeon Geum, Yeaseul Kim, Rona L. Thompson, Jens Mühle, Peter K. Salameh, Christina M. Harth, Kieran M. Stanley, Simon O'Doherty, Paul J. Fraser, Peter G. Simmonds, Paul B. Krummel, Ray F. Weiss, Ronald G. Prinn, and Sunyoung Park
Atmos. Chem. Phys., 23, 9401–9411, https://doi.org/10.5194/acp-23-9401-2023, https://doi.org/10.5194/acp-23-9401-2023, 2023
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Based on atmospheric HFC-23 observations, the first estimate of post-CDM HFC-23 emissions in eastern Asia for 2008–2019 shows that these emissions contribute significantly to the global emissions rise. The observation-derived emissions were much larger than the bottom-up estimates expected to approach zero after 2015 due to national abatement activities. These discrepancies could be attributed to unsuccessful factory-level HFC-23 abatement and inaccurate quantification of emission reductions.
Alison L. Redington, Alistair J. Manning, Stephan Henne, Francesco Graziosi, Luke M. Western, Jgor Arduini, Anita L. Ganesan, Christina M. Harth, Michela Maione, Jens Mühle, Simon O'Doherty, Joseph Pitt, Stefan Reimann, Matthew Rigby, Peter K. Salameh, Peter G. Simmonds, T. Gerard Spain, Kieran Stanley, Martin K. Vollmer, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 23, 7383–7398, https://doi.org/10.5194/acp-23-7383-2023, https://doi.org/10.5194/acp-23-7383-2023, 2023
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Chlorofluorocarbons (CFCs) were used in Europe pre-1990, damaging the stratospheric ozone layer. Legislation has controlled production and use, and global emissions have decreased sharply. The global rate of decline in CFC-11 recently slowed and was partly attributed to illegal emission in eastern China. This study concludes that emissions of CFC-11 in western Europe have not contributed to the unexplained part of the global increase in CFC-11 observed in the last decade.
Emily Dowd, Chris Wilson, Martyn P. Chipperfield, Emanuel Gloor, Alistair Manning, and Ruth Doherty
Atmos. Chem. Phys., 23, 7363–7382, https://doi.org/10.5194/acp-23-7363-2023, https://doi.org/10.5194/acp-23-7363-2023, 2023
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Surface observations of methane show that the seasonal cycle amplitude (SCA) of methane is decreasing in the northern high latitudes (NHLs) but increased globally (1995–2020). The NHL decrease is counterintuitive, as we expect the SCA to increase with increasing concentrations. We use a chemical transport model to investigate changes in SCA in the NHLs. We find well-mixed methane and changes in emissions from Canada, the Middle East, and Europe are the largest contributors to the SCA in NHLs.
Peter Joyce, Cristina Ruiz Villena, Yahui Huang, Alex Webb, Manuel Gloor, Fabien H. Wagner, Martyn P. Chipperfield, Rocío Barrio Guilló, Chris Wilson, and Hartmut Boesch
Atmos. Meas. Tech., 16, 2627–2640, https://doi.org/10.5194/amt-16-2627-2023, https://doi.org/10.5194/amt-16-2627-2023, 2023
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Methane emissions are responsible for a lot of the warming caused by the greenhouse effect, much of which comes from a small number of point sources. We can identify methane point sources by analysing satellite data, but it requires a lot of time invested by experts and is prone to very high errors. Here, we produce a neural network that can automatically identify methane point sources and estimate the mass of methane that is being released per hour and are able to do so with far smaller errors.
Antonio G. Bruno, Jeremy J. Harrison, Martyn P. Chipperfield, David P. Moore, Richard J. Pope, Christopher Wilson, Emmanuel Mahieu, and Justus Notholt
Atmos. Chem. Phys., 23, 4849–4861, https://doi.org/10.5194/acp-23-4849-2023, https://doi.org/10.5194/acp-23-4849-2023, 2023
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A 3-D chemical transport model, TOMCAT; satellite data; and ground-based observations have been used to investigate hydrogen cyanide (HCN) variability. We found that the oxidation by O(1D) drives the HCN loss in the middle stratosphere and the currently JPL-recommended OH reaction rate overestimates HCN atmospheric loss. We also evaluated two different ocean uptake schemes. We found them to be unrealistic, and we need to scale these schemes to obtain good agreement with HCN observations.
Elena Fillola, Raul Santos-Rodriguez, Alistair Manning, Simon O'Doherty, and Matt Rigby
Geosci. Model Dev., 16, 1997–2009, https://doi.org/10.5194/gmd-16-1997-2023, https://doi.org/10.5194/gmd-16-1997-2023, 2023
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Lagrangian particle dispersion models are used extensively for the estimation of greenhouse gas (GHG) fluxes using atmospheric observations. However, these models do not scale well as data volumes increase. Here, we develop a proof-of-concept machine learning emulator that can produce outputs similar to those of the dispersion model, but 50 000 times faster, using only meteorological inputs. This works demonstrates the potential of machine learning to accelerate GHG estimations across the globe.
Ana Maria Roxana Petrescu, Chunjing Qiu, Matthew J. McGrath, Philippe Peylin, Glen P. Peters, Philippe Ciais, Rona L. Thompson, Aki Tsuruta, Dominik Brunner, Matthias Kuhnert, Bradley Matthews, Paul I. Palmer, Oksana Tarasova, Pierre Regnier, Ronny Lauerwald, David Bastviken, Lena Höglund-Isaksson, Wilfried Winiwarter, Giuseppe Etiope, Tuula Aalto, Gianpaolo Balsamo, Vladislav Bastrikov, Antoine Berchet, Patrick Brockmann, Giancarlo Ciotoli, Giulia Conchedda, Monica Crippa, Frank Dentener, Christine D. Groot Zwaaftink, Diego Guizzardi, Dirk Günther, Jean-Matthieu Haussaire, Sander Houweling, Greet Janssens-Maenhout, Massaer Kouyate, Adrian Leip, Antti Leppänen, Emanuele Lugato, Manon Maisonnier, Alistair J. Manning, Tiina Markkanen, Joe McNorton, Marilena Muntean, Gabriel D. Oreggioni, Prabir K. Patra, Lucia Perugini, Isabelle Pison, Maarit T. Raivonen, Marielle Saunois, Arjo J. Segers, Pete Smith, Efisio Solazzo, Hanqin Tian, Francesco N. Tubiello, Timo Vesala, Guido R. van der Werf, Chris Wilson, and Sönke Zaehle
Earth Syst. Sci. Data, 15, 1197–1268, https://doi.org/10.5194/essd-15-1197-2023, https://doi.org/10.5194/essd-15-1197-2023, 2023
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This study updates the state-of-the-art scientific overview of CH4 and N2O emissions in the EU27 and UK in Petrescu et al. (2021a). Yearly updates are needed to improve the different respective approaches and to inform on the development of formal verification systems. It integrates the most recent emission inventories, process-based model and regional/global inversions, comparing them with UNFCCC national GHG inventories, in support to policy to facilitate real-time verification procedures.
Michael N. Dyonisius, Vasilii V. Petrenko, Andrew M. Smith, Benjamin Hmiel, Peter D. Neff, Bin Yang, Quan Hua, Jochen Schmitt, Sarah A. Shackleton, Christo Buizert, Philip F. Place, James A. Menking, Ross Beaudette, Christina Harth, Michael Kalk, Heidi A. Roop, Bernhard Bereiter, Casey Armanetti, Isaac Vimont, Sylvia Englund Michel, Edward J. Brook, Jeffrey P. Severinghaus, Ray F. Weiss, and Joseph R. McConnell
The Cryosphere, 17, 843–863, https://doi.org/10.5194/tc-17-843-2023, https://doi.org/10.5194/tc-17-843-2023, 2023
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Cosmic rays that enter the atmosphere produce secondary particles which react with surface minerals to produce radioactive nuclides. These nuclides are often used to constrain Earth's surface processes. However, the production rates from muons are not well constrained. We measured 14C in ice with a well-known exposure history to constrain the production rates from muons. 14C production in ice is analogous to quartz, but we obtain different production rates compared to commonly used estimates.
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.
Robert J. Parker, Chris Wilson, Edward Comyn-Platt, Garry Hayman, Toby R. Marthews, A. Anthony Bloom, Mark F. Lunt, Nicola Gedney, Simon J. Dadson, Joe McNorton, Neil Humpage, Hartmut Boesch, Martyn P. Chipperfield, Paul I. Palmer, and Dai Yamazaki
Biogeosciences, 19, 5779–5805, https://doi.org/10.5194/bg-19-5779-2022, https://doi.org/10.5194/bg-19-5779-2022, 2022
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Wetlands are the largest natural source of methane, one of the most important climate gases. The JULES land surface model simulates these emissions. We use satellite data to evaluate how well JULES reproduces the methane seasonal cycle over different tropical wetlands. It performs well for most regions; however, it struggles for some African wetlands influenced heavily by river flooding. We explain the reasons for these deficiencies and highlight how future development will improve these areas.
Sourish Basu, Xin Lan, Edward Dlugokencky, Sylvia Michel, Stefan Schwietzke, John B. Miller, Lori Bruhwiler, Youmi Oh, Pieter P. Tans, Francesco Apadula, Luciana V. Gatti, Armin Jordan, Jaroslaw Necki, Motoki Sasakawa, Shinji Morimoto, Tatiana Di Iorio, Haeyoung Lee, Jgor Arduini, and Giovanni Manca
Atmos. Chem. Phys., 22, 15351–15377, https://doi.org/10.5194/acp-22-15351-2022, https://doi.org/10.5194/acp-22-15351-2022, 2022
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Atmospheric methane (CH4) has been growing steadily since 2007 for reasons that are not well understood. Here we determine sources of methane using a technique informed by atmospheric measurements of CH4 and its isotopologue 13CH4. Measurements of 13CH4 provide for better separation of microbial, fossil, and fire sources of methane than CH4 measurements alone. Compared to previous assessments such as the Global Carbon Project, we find a larger microbial contribution to the post-2007 increase.
Markus Jesswein, Rafael P. Fernandez, Lucas Berná, Alfonso Saiz-Lopez, Jens-Uwe Grooß, Ryan Hossaini, Eric C. Apel, Rebecca S. Hornbrook, Elliot L. Atlas, Donald R. Blake, Stephen Montzka, Timo Keber, Tanja Schuck, Thomas Wagenhäuser, and Andreas Engel
Atmos. Chem. Phys., 22, 15049–15070, https://doi.org/10.5194/acp-22-15049-2022, https://doi.org/10.5194/acp-22-15049-2022, 2022
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This study presents the global and seasonal distribution of the two major brominated short-lived substances CH2Br2 and CHBr3 in the upper troposphere and lower stratosphere based on observations from several aircraft campaigns. They show similar seasonality for both hemispheres, except in the respective hemispheric autumn lower stratosphere. A comparison with the TOMCAT and CAM-Chem models shows good agreement in the annual mean but larger differences in the seasonal consideration.
Peter Bergamaschi, Arjo Segers, Dominik Brunner, Jean-Matthieu Haussaire, Stephan Henne, Michel Ramonet, Tim Arnold, Tobias Biermann, Huilin Chen, Sebastien Conil, Marc Delmotte, Grant Forster, Arnoud Frumau, Dagmar Kubistin, Xin Lan, Markus Leuenberger, Matthias Lindauer, Morgan Lopez, Giovanni Manca, Jennifer Müller-Williams, Simon O'Doherty, Bert Scheeren, Martin Steinbacher, Pamela Trisolino, Gabriela Vítková, and Camille Yver Kwok
Atmos. Chem. Phys., 22, 13243–13268, https://doi.org/10.5194/acp-22-13243-2022, https://doi.org/10.5194/acp-22-13243-2022, 2022
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We present a novel high-resolution inverse modelling system, "FLEXVAR", and its application for the inverse modelling of European CH4 emissions in 2018. The new system combines a high spatial resolution of 7 km x 7 km with a variational data assimilation technique, which allows CH4 emissions to be optimized from individual model grid cells. The high resolution allows the observations to be better reproduced, while the derived emissions show overall good consistency with two existing models.
Angharad C. Stell, Michael Bertolacci, Andrew Zammit-Mangion, Matthew Rigby, Paul J. Fraser, Christina M. Harth, Paul B. Krummel, Xin Lan, Manfredi Manizza, Jens Mühle, Simon O'Doherty, Ronald G. Prinn, Ray F. Weiss, Dickon Young, and Anita L. Ganesan
Atmos. Chem. Phys., 22, 12945–12960, https://doi.org/10.5194/acp-22-12945-2022, https://doi.org/10.5194/acp-22-12945-2022, 2022
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Nitrous oxide is a potent greenhouse gas and ozone-depleting substance, whose atmospheric abundance has risen throughout the contemporary record. In this work, we carry out the first global hierarchical Bayesian inversion to solve for nitrous oxide emissions. We derive increasing global nitrous oxide emissions over 2011–2020, which are mainly driven by emissions between 0° and 30°N, with the highest emissions recorded in 2020.
Maria Paula Pérez-Peña, Jenny A. Fisher, Dylan B. Millet, Hisashi Yashiro, Ray L. Langenfelds, Paul B. Krummel, and Scott H. Kable
Atmos. Chem. Phys., 22, 12367–12386, https://doi.org/10.5194/acp-22-12367-2022, https://doi.org/10.5194/acp-22-12367-2022, 2022
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We used two atmospheric models to test the implications of previously unexplored aldehyde photochemistry on the atmospheric levels of molecular hydrogen (H2). We showed that the new photochemistry from aldehydes produces more H2 over densely forested areas. Compared to the rest of the world, it is over these forested regions where the produced H2 is more likely to be removed. The results highlight that other processes that contribute to atmospheric H2 levels should be studied further.
Ewa M. Bednarz, Ryan Hossaini, Martyn P. Chipperfield, N. Luke Abraham, and Peter Braesicke
Atmos. Chem. Phys., 22, 10657–10676, https://doi.org/10.5194/acp-22-10657-2022, https://doi.org/10.5194/acp-22-10657-2022, 2022
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Atmospheric impacts of chlorinated very short-lived substances (Cl-VSLS) over the first two decades of the 21st century are assessed using the UM-UKCA chemistry–climate model. Stratospheric input of Cl from Cl-VSLS is estimated at ~130 ppt in 2019. The use of model set-up with constrained meteorology significantly increases the abundance of Cl-VSLS in the lower stratosphere relative to the free-running set-up. The growth in Cl-VSLS emissions significantly impacted recent HCl and COCl2 trends.
Yajuan Li, Sandip S. Dhomse, Martyn P. Chipperfield, Wuhu Feng, Andreas Chrysanthou, Yuan Xia, and Dong Guo
Atmos. Chem. Phys., 22, 10635–10656, https://doi.org/10.5194/acp-22-10635-2022, https://doi.org/10.5194/acp-22-10635-2022, 2022
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Chemical transport models forced with (re)analysis meteorological fields are ideally suited for interpreting the influence of important physical processes on the ozone variability. We use TOMCAT forced by ECMWF ERA-Interim and ERA5 reanalysis data sets to investigate the effects of reanalysis forcing fields on ozone changes. Our results show that models forced by ERA5 reanalyses may not yet be capable of reproducing observed changes in stratospheric ozone, particularly in the lower stratosphere.
Matilda A. Pimlott, Richard J. Pope, Brian J. Kerridge, Barry G. Latter, Diane S. Knappett, Dwayne E. Heard, Lucy J. Ventress, Richard Siddans, Wuhu Feng, and Martyn P. Chipperfield
Atmos. Chem. Phys., 22, 10467–10488, https://doi.org/10.5194/acp-22-10467-2022, https://doi.org/10.5194/acp-22-10467-2022, 2022
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We present a new method to derive global information of the hydroxyl radical (OH), an important atmospheric oxidant. OH controls the lifetime of trace gases important to air quality and climate. We use satellite observations of ozone, carbon monoxide, methane and water vapour in a simple expression to derive OH around 3–4 km altitude. The derived OH compares well to model and aircraft OH data. We then apply the method to 10 years of satellite data to study the inter-annual variability of OH.
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.
Toby R. Marthews, Simon J. Dadson, Douglas B. Clark, Eleanor M. Blyth, Garry D. Hayman, Dai Yamazaki, Olivia R. E. Becher, Alberto Martínez-de la Torre, Catherine Prigent, and Carlos Jiménez
Hydrol. Earth Syst. Sci., 26, 3151–3175, https://doi.org/10.5194/hess-26-3151-2022, https://doi.org/10.5194/hess-26-3151-2022, 2022
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Reliable data on global inundated areas remain uncertain. By matching a leading global data product on inundation extents (GIEMS) against predictions from a global hydrodynamic model (CaMa-Flood), we found small but consistent and non-random biases in well-known tropical wetlands (Sudd, Pantanal, Amazon and Congo). These result from known limitations in the data and the models used, which shows us how to improve our ability to make critical predictions of inundation events in the future.
Guus J. M. Velders, John S. Daniel, Stephen A. Montzka, Isaac Vimont, Matthew Rigby, Paul B. Krummel, Jens Muhle, Simon O'Doherty, Ronald G. Prinn, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 22, 6087–6101, https://doi.org/10.5194/acp-22-6087-2022, https://doi.org/10.5194/acp-22-6087-2022, 2022
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The emissions of hydrofluorocarbons (HFCs) have increased significantly in the past as a result of the phasing out of ozone-depleting substances. Observations indicate that HFCs are used much less in certain refrigeration applications than previously projected. Current policies are projected to reduce emissions and the surface temperature contribution of HFCs from 0.28–0.44 °C to 0.14–0.31 °C in 2100. The Kigali Amendment is projected to reduce the contributions further to 0.04 °C in 2100.
Haklim Choi, Mi-Kyung Park, Paul J. Fraser, Hyeri Park, Sohyeon Geum, Jens Mühle, Jooil Kim, Ian Porter, Peter K. Salameh, Christina M. Harth, Bronwyn L. Dunse, Paul B. Krummel, Ray F. Weiss, Simon O'Doherty, Dickon Young, and Sunyoung Park
Atmos. Chem. Phys., 22, 5157–5173, https://doi.org/10.5194/acp-22-5157-2022, https://doi.org/10.5194/acp-22-5157-2022, 2022
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We observed 12-year continuous CH3Br pollution signals at Gosan and estimated anthropogenic CH3Br emissions in eastern China. The analysis revealed a significant discrepancy between top-down estimates and the bottom-up emissions from the fumigation usage reported to the United Nations Environment Programme, likely due to unreported or inaccurately reported fumigation usage. This result provides information to monitor international compliance with the Montreal Protocol.
Beatriz M. Monge-Sanz, Alessio Bozzo, Nicholas Byrne, Martyn P. Chipperfield, Michail Diamantakis, Johannes Flemming, Lesley J. Gray, Robin J. Hogan, Luke Jones, Linus Magnusson, Inna Polichtchouk, Theodore G. Shepherd, Nils Wedi, and Antje Weisheimer
Atmos. Chem. Phys., 22, 4277–4302, https://doi.org/10.5194/acp-22-4277-2022, https://doi.org/10.5194/acp-22-4277-2022, 2022
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The stratosphere is emerging as one of the keys to improve tropospheric weather and climate predictions. This study provides evidence of the role the stratospheric ozone layer plays in improving weather predictions at different timescales. Using a new ozone modelling approach suitable for high-resolution global models that provide operational forecasts from days to seasons, we find significant improvements in stratospheric meteorological fields and stratosphere–troposphere coupling.
Richard J. Pope, Rebecca Kelly, Eloise A. Marais, Ailish M. Graham, Chris Wilson, Jeremy J. Harrison, Savio J. A. Moniz, Mohamed Ghalaieny, Steve R. Arnold, and Martyn P. Chipperfield
Atmos. Chem. Phys., 22, 4323–4338, https://doi.org/10.5194/acp-22-4323-2022, https://doi.org/10.5194/acp-22-4323-2022, 2022
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Nitrogen oxides (NOx) are potent air pollutants which directly impact on human health. In this study, we use satellite nitrogen dioxide (NO2) data to evaluate the spatial distribution and temporal evolution of the UK official NOx emissions inventory, with reasonable agreement. We also derived satellite-based NOx emissions for several UK cities. In the case of London and Birmingham, the NAEI NOx emissions are potentially too low by >50%.
Piera Raspollini, Enrico Arnone, Flavio Barbara, Massimo Bianchini, Bruno Carli, Simone Ceccherini, Martyn P. Chipperfield, Angelika Dehn, Stefano Della Fera, Bianca Maria Dinelli, Anu Dudhia, Jean-Marie Flaud, Marco Gai, Michael Kiefer, Manuel López-Puertas, David P. Moore, Alessandro Piro, John J. Remedios, Marco Ridolfi, Harjinder Sembhi, Luca Sgheri, and Nicola Zoppetti
Atmos. Meas. Tech., 15, 1871–1901, https://doi.org/10.5194/amt-15-1871-2022, https://doi.org/10.5194/amt-15-1871-2022, 2022
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The MIPAS instrument onboard the ENVISAT satellite provided 10 years of measurements of the atmospheric emission al limb that allow for the retrieval of latitude- and altitude-resolved atmospheric composition. We describe the improvements implemented in the retrieval algorithm used for the full mission reanalysis, which allows for the generation of the global distributions of 21 atmospheric constituents plus temperature with increased accuracy with respect to previously generated data.
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.
Sandip S. Dhomse, Martyn P. Chipperfield, Wuhu Feng, Ryan Hossaini, Graham W. Mann, Michelle L. Santee, and Mark Weber
Atmos. Chem. Phys., 22, 903–916, https://doi.org/10.5194/acp-22-903-2022, https://doi.org/10.5194/acp-22-903-2022, 2022
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Solar flux variations associated with 11-year sunspot cycle is believed to exert important external climate forcing. As largest variations occur at shorter wavelengths such as ultra-violet part of the solar spectrum, associated changes in stratospheric ozone are thought to provide direct evidence for solar climate interaction. Until now, most of the studies reported double-peak structured solar cycle signal (SCS), but relatively new satellite data suggest only single-peak-structured SCS.
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.
Sandip S. Dhomse, Carlo Arosio, Wuhu Feng, Alexei Rozanov, Mark Weber, and Martyn P. Chipperfield
Earth Syst. Sci. Data, 13, 5711–5729, https://doi.org/10.5194/essd-13-5711-2021, https://doi.org/10.5194/essd-13-5711-2021, 2021
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High-quality long-term ozone profile data sets are key to estimating short- and long-term ozone variability. Almost all the satellite (and chemical model) data sets show some kind of bias with respect to each other. This is because of differences in measurement methodologies as well as simplified processes in the models. We use satellite data sets and chemical model output to generate 42 years of ozone profile data sets using a random-forest machine-learning algorithm that is named ML-TOMCAT.
Paul D. Hamer, Virginie Marécal, Ryan Hossaini, Michel Pirre, Gisèle Krysztofiak, Franziska Ziska, Andreas Engel, Stephan Sala, Timo Keber, Harald Bönisch, Elliot Atlas, Kirstin Krüger, Martyn Chipperfield, Valery Catoire, Azizan A. Samah, Marcel Dorf, Phang Siew Moi, Hans Schlager, and Klaus Pfeilsticker
Atmos. Chem. Phys., 21, 16955–16984, https://doi.org/10.5194/acp-21-16955-2021, https://doi.org/10.5194/acp-21-16955-2021, 2021
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Bromoform is a stratospheric ozone-depleting gas released by seaweed and plankton transported to the stratosphere via convection in the tropics. We study the chemical interactions of bromoform and its derivatives within convective clouds using a cloud-scale model and observations. Our findings are that soluble bromine gases are efficiently washed out and removed within the convective clouds and that most bromine is transported vertically to the upper troposphere in the form of bromoform.
Vilma Kangasaho, Aki Tsuruta, Leif Backman, Pyry Mäkinen, Sander Houweling, Arjo Segers, Maarten Krol, Ed Dlugokencky, Sylvia Michel, James White, and Tuula Aalto
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-843, https://doi.org/10.5194/acp-2021-843, 2021
Revised manuscript not accepted
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Understanding the composition of carbon isotopes can help to better understand the changes in methane budgets. This study investigates how methane sources affect the seasonal cycle of the methane carbon-13 isotope during 2000–2012 using an atmospheric transport model. We found that emissions from both anthropogenic and natural sources contribute. The findings raise a need to revise the magnitudes, proportion, and seasonal cycles of anthropogenic sources and northern wetland emissions.
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.
Meike K. Rotermund, Vera Bense, Martyn P. Chipperfield, Andreas Engel, Jens-Uwe Grooß, Peter Hoor, Tilman Hüneke, Timo Keber, Flora Kluge, Benjamin Schreiner, Tanja Schuck, Bärbel Vogel, Andreas Zahn, and Klaus Pfeilsticker
Atmos. Chem. Phys., 21, 15375–15407, https://doi.org/10.5194/acp-21-15375-2021, https://doi.org/10.5194/acp-21-15375-2021, 2021
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Airborne total bromine (Brtot) and tracer measurements suggest Brtot-rich air masses persistently protruded into the lower stratosphere (LS), creating a high Brtot region over the North Atlantic in fall 2017. The main source is via isentropic transport by the Asian monsoon and to a lesser extent transport across the extratropical tropopause as quantified by a Lagrange model. The transport of Brtot via Central American hurricanes is also observed. Lastly, the impact of Brtot on LS O3 is assessed.
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.
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.
Yi Yin, Frederic Chevallier, Philippe Ciais, Philippe Bousquet, Marielle Saunois, Bo Zheng, John Worden, A. Anthony Bloom, Robert J. Parker, Daniel J. Jacob, Edward J. Dlugokencky, and Christian Frankenberg
Atmos. Chem. Phys., 21, 12631–12647, https://doi.org/10.5194/acp-21-12631-2021, https://doi.org/10.5194/acp-21-12631-2021, 2021
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The growth of methane, the second-most important anthropogenic greenhouse gas after carbon dioxide, has been accelerating in recent years. Using an ensemble of multi-tracer atmospheric inversions constrained by surface or satellite observations, we show that global methane emissions increased by nearly 1 % per year from 2010–2017, with leading contributions from the tropics and East Asia.
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.
Chris Wilson, Martyn P. Chipperfield, Manuel Gloor, Robert J. Parker, Hartmut Boesch, Joey McNorton, Luciana V. Gatti, John B. Miller, Luana S. Basso, and Sarah A. Monks
Atmos. Chem. Phys., 21, 10643–10669, https://doi.org/10.5194/acp-21-10643-2021, https://doi.org/10.5194/acp-21-10643-2021, 2021
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Methane (CH4) is an important greenhouse gas emitted from wetlands like those found in the basin of the Amazon River. Using an atmospheric model and observations from GOSAT, we quantified CH4 emissions from Amazonia during the previous decade. We found that the largest emissions came from a region in the eastern basin and that emissions there were rising faster than in other areas of South America. This finding was supported by CH4 observations made on aircraft within the basin.
Ana Maria Roxana Petrescu, Chunjing Qiu, Philippe Ciais, Rona L. Thompson, Philippe Peylin, Matthew J. McGrath, Efisio Solazzo, Greet Janssens-Maenhout, Francesco N. Tubiello, Peter Bergamaschi, Dominik Brunner, Glen P. Peters, Lena Höglund-Isaksson, Pierre Regnier, Ronny Lauerwald, David Bastviken, Aki Tsuruta, Wilfried Winiwarter, Prabir K. Patra, Matthias Kuhnert, Gabriel D. Oreggioni, Monica Crippa, Marielle Saunois, Lucia Perugini, Tiina Markkanen, Tuula Aalto, Christine D. Groot Zwaaftink, Hanqin Tian, Yuanzhi Yao, Chris Wilson, Giulia Conchedda, Dirk Günther, Adrian Leip, Pete Smith, Jean-Matthieu Haussaire, Antti Leppänen, Alistair J. Manning, Joe McNorton, Patrick Brockmann, and Albertus Johannes Dolman
Earth Syst. Sci. Data, 13, 2307–2362, https://doi.org/10.5194/essd-13-2307-2021, https://doi.org/10.5194/essd-13-2307-2021, 2021
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This study is topical and provides a state-of-the-art scientific overview of data availability from bottom-up and top-down CH4 and N2O emissions in the EU27 and UK. The data integrate recent emission inventories with process-based model data and regional/global inversions for the European domain, aiming at reconciling them with official country-level UNFCCC national GHG inventories in support to policy and to facilitate real-time verification procedures.
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.
Garry D. Hayman, Edward Comyn-Platt, Chris Huntingford, Anna B. Harper, Tom Powell, Peter M. Cox, William Collins, Christopher Webber, Jason Lowe, Stephen Sitch, Joanna I. House, Jonathan C. Doelman, Detlef P. van Vuuren, Sarah E. Chadburn, Eleanor Burke, and Nicola Gedney
Earth Syst. Dynam., 12, 513–544, https://doi.org/10.5194/esd-12-513-2021, https://doi.org/10.5194/esd-12-513-2021, 2021
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We model greenhouse gas emission scenarios consistent with limiting global warming to either 1.5 or 2 °C above pre-industrial levels. We quantify the effectiveness of methane emission control and land-based mitigation options regionally. Our results highlight the importance of reducing methane emissions for realistic emission pathways that meet the global warming targets. For land-based mitigation, growing bioenergy crops on existing agricultural land is preferable to replacing forests.
Akash Biswal, Vikas Singh, Shweta Singh, Amit P. Kesarkar, Khaiwal Ravindra, Ranjeet S. Sokhi, Martyn P. Chipperfield, Sandip S. Dhomse, Richard J. Pope, Tanbir Singh, and Suman Mor
Atmos. Chem. Phys., 21, 5235–5251, https://doi.org/10.5194/acp-21-5235-2021, https://doi.org/10.5194/acp-21-5235-2021, 2021
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Satellite and surface observations show a reduction in NO2 levels over India during the lockdown compared to business-as-usual years. A substantial reduction, proportional to the population, was observed over the urban areas. The changes in NO2 levels at the surface during the lockdown appear to be present in the satellite observations. However, TROPOMI showed a better correlation with surface NO2 and was more sensitive to the changes than OMI because of the finer resolution.
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.
Julia Drewer, Melissa M. Leduning, Robert I. Griffiths, Tim Goodall, Peter E. Levy, Nicholas Cowan, Edward Comynn-Platt, Garry Hayman, Justin Sentian, Noreen Majalap, and Ute M. Skiba
Biogeosciences, 18, 1559–1575, https://doi.org/10.5194/bg-18-1559-2021, https://doi.org/10.5194/bg-18-1559-2021, 2021
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In Southeast Asia, oil palm plantations have largely replaced tropical forests. The impact of this shift in land use on greenhouse gas fluxes and soil microbial communities remains uncertain. We have found emission rates of the potent greenhouse gas nitrous oxide on mineral soil to be higher from oil palm plantations than logged forest over a 2-year study and concluded that emissions have increased over the last 42 years in Sabah, with the proportion of emissions from plantations increasing.
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.
Shamil Maksyutov, Tomohiro Oda, Makoto Saito, Rajesh Janardanan, Dmitry Belikov, Johannes W. Kaiser, Ruslan Zhuravlev, Alexander Ganshin, Vinu K. Valsala, Arlyn Andrews, Lukasz Chmura, Edward Dlugokencky, László Haszpra, Ray L. Langenfelds, Toshinobu Machida, Takakiyo Nakazawa, Michel Ramonet, Colm Sweeney, and Douglas Worthy
Atmos. Chem. Phys., 21, 1245–1266, https://doi.org/10.5194/acp-21-1245-2021, https://doi.org/10.5194/acp-21-1245-2021, 2021
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In order to improve the top-down estimation of the anthropogenic greenhouse gas emissions, a high-resolution inverse modelling technique was developed for applications to global transport modelling of carbon dioxide and other greenhouse gases. A coupled Eulerian–Lagrangian transport model and its adjoint are combined with surface fluxes at 0.1° resolution to provide high-resolution forward simulation and inverse modelling of surface fluxes accounting for signals from emission hot spots.
Susan S. Kulawik, John R. Worden, Vivienne H. Payne, Dejian Fu, Steven C. Wofsy, Kathryn McKain, Colm Sweeney, Bruce C. Daube Jr., Alan Lipton, Igor Polonsky, Yuguang He, Karen E. Cady-Pereira, Edward J. Dlugokencky, Daniel J. Jacob, and Yi Yin
Atmos. Meas. Tech., 14, 335–354, https://doi.org/10.5194/amt-14-335-2021, https://doi.org/10.5194/amt-14-335-2021, 2021
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This paper shows comparisons of a new single-footprint methane product from the AIRS satellite to aircraft-based observations. We show that this AIRS methane product provides useful information to study seasonal and global methane trends of this important greenhouse gas.
Tea Thum, Julia E. M. S. Nabel, Aki Tsuruta, Tuula Aalto, Edward J. Dlugokencky, Jari Liski, Ingrid T. Luijkx, Tiina Markkanen, Julia Pongratz, Yukio Yoshida, and Sönke Zaehle
Biogeosciences, 17, 5721–5743, https://doi.org/10.5194/bg-17-5721-2020, https://doi.org/10.5194/bg-17-5721-2020, 2020
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Global vegetation models are important tools in estimating the impacts of global climate change. The fate of soil carbon is of the upmost importance as its emissions will enhance the atmospheric carbon dioxide concentration. To evaluate the skill of global vegetation models to model the soil carbon and its responses to environmental factors, it is important to use different data sources. We evaluated two different soil carbon models by using atmospheric carbon dioxide concentrations.
Robert J. Parker, Chris Wilson, A. Anthony Bloom, Edward Comyn-Platt, Garry Hayman, Joe McNorton, Hartmut Boesch, and Martyn P. Chipperfield
Biogeosciences, 17, 5669–5691, https://doi.org/10.5194/bg-17-5669-2020, https://doi.org/10.5194/bg-17-5669-2020, 2020
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Wetlands contribute the largest uncertainty to the atmospheric methane budget. WetCHARTs is a simple, data-driven model that estimates wetland emissions using observations of precipitation and temperature. We perform the first detailed evaluation of WetCHARTs against satellite data and find it performs well in reproducing the observed wetland methane seasonal cycle for the majority of wetland regions. In regions where it performs poorly, we highlight incorrect wetland extent as a key reason.
Sandip S. Dhomse, Graham W. Mann, Juan Carlos Antuña Marrero, Sarah E. Shallcross, Martyn P. Chipperfield, Kenneth S. Carslaw, Lauren Marshall, N. Luke Abraham, and Colin E. Johnson
Atmos. Chem. Phys., 20, 13627–13654, https://doi.org/10.5194/acp-20-13627-2020, https://doi.org/10.5194/acp-20-13627-2020, 2020
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We confirm downward adjustment of SO2 emission to simulate the Pinatubo aerosol cloud with aerosol microphysics models. Similar adjustment is also needed to simulate the El Chichón and Agung volcanic cloud, indicating potential missing removal or vertical redistribution process in models. Important inhomogeneities in the CMIP6 forcing datasets after Agung and El Chichón eruptions are difficult to reconcile. Quasi-biennial oscillation plays an important role in modifying stratospheric warming.
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.
Yuanhong Zhao, Marielle Saunois, Philippe Bousquet, Xin Lin, Antoine Berchet, Michaela I. Hegglin, Josep G. Canadell, Robert B. Jackson, Makoto Deushi, Patrick Jöckel, Douglas Kinnison, Ole Kirner, Sarah Strode, Simone Tilmes, Edward J. Dlugokencky, and Bo Zheng
Atmos. Chem. Phys., 20, 13011–13022, https://doi.org/10.5194/acp-20-13011-2020, https://doi.org/10.5194/acp-20-13011-2020, 2020
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Decadal trends and variations in OH are critical for understanding atmospheric CH4 evolution. We quantify the impacts of OH trends and variations on the CH4 budget by conducting CH4 inversions on a decadal scale with an ensemble of OH fields. We find the negative OH anomalies due to enhanced fires can reduce the optimized CH4 emissions by up to 10 Tg yr−1 during El Niño years and the positive OH trend from 1986 to 2010 results in a ∼ 23 Tg yr−1 additional increase in optimized CH4 emissions.
Benjamin Birner, Martyn P. Chipperfield, Eric J. Morgan, Britton B. Stephens, Marianna Linz, Wuhu Feng, Chris Wilson, Jonathan D. Bent, Steven C. Wofsy, Jeffrey Severinghaus, and Ralph F. Keeling
Atmos. Chem. Phys., 20, 12391–12408, https://doi.org/10.5194/acp-20-12391-2020, https://doi.org/10.5194/acp-20-12391-2020, 2020
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With new high-precision observations from nine aircraft campaigns and 3-D chemical transport modeling, we show that the argon-to-nitrogen ratio (Ar / N2) in the lowermost stratosphere provides a useful constraint on the “age of air” (the time elapsed since entry of an air parcel into the stratosphere). Therefore, Ar / N2 in combination with traditional age-of-air indicators, such as CO2 and N2O, could provide new insights into atmospheric mixing and transport.
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.
Haeyoung Lee, Edward J. Dlugokencky, Jocelyn C. Turnbull, Sepyo Lee, Scott J. Lehman, John B. Miller, Gabrielle Pétron, Jeong-Sik Lim, Gang-Woong Lee, Sang-Sam Lee, and Young-San Park
Atmos. Chem. Phys., 20, 12033–12045, https://doi.org/10.5194/acp-20-12033-2020, https://doi.org/10.5194/acp-20-12033-2020, 2020
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To understand South Korea's CO2 emissions and sinks as well as those of the surrounding region, we used flask-air samples collected for 2 years at Anmyeondo (36.53° N, 126.32° E; 46 m a.s.l.), South Korea, for analysis of observed 14C in atmospheric CO2 as a tracer of fossil fuel CO2 contribution (Cff). Here, we showed our observation result of 14C and Cff. SF6 and CO can be good proxies of Cff in this study, and the ratio of CO to Cff was compared to a bottom-up inventory.
Matthew J. Rowlinson, Alexandru Rap, Douglas S. Hamilton, Richard J. Pope, Stijn Hantson, Steve R. Arnold, Jed O. Kaplan, Almut Arneth, Martyn P. Chipperfield, Piers M. Forster, and Lars Nieradzik
Atmos. Chem. Phys., 20, 10937–10951, https://doi.org/10.5194/acp-20-10937-2020, https://doi.org/10.5194/acp-20-10937-2020, 2020
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Tropospheric ozone is an important greenhouse gas which contributes to anthropogenic climate change; however, the effect of human emissions is uncertain because pre-industrial ozone concentrations are not well understood. We use revised inventories of pre-industrial natural emissions to estimate the human contribution to changes in tropospheric ozone. We find that tropospheric ozone radiative forcing is up to 34 % lower when using improved pre-industrial biomass burning and vegetation emissions.
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.
Yuanhong Zhao, Marielle Saunois, Philippe Bousquet, Xin Lin, Antoine Berchet, Michaela I. Hegglin, Josep G. Canadell, Robert B. Jackson, Edward J. Dlugokencky, Ray L. Langenfelds, Michel Ramonet, Doug Worthy, and Bo Zheng
Atmos. Chem. Phys., 20, 9525–9546, https://doi.org/10.5194/acp-20-9525-2020, https://doi.org/10.5194/acp-20-9525-2020, 2020
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The hydroxyl radical (OH), which is the dominant sink of methane (CH4), plays a key role in closing the global methane budget. This study quantifies how uncertainties in the hydroxyl radical can influence top-down estimates of CH4 emissions based on 4D Bayesian inversions with different OH fields and the same surface observations. We show that uncertainties in CH4 emissions driven by different OH fields are comparable to the uncertainties given by current bottom-up and top-down estimations.
Yajuan Li, Martyn P. Chipperfield, Wuhu Feng, Sandip S. Dhomse, Richard J. Pope, Faquan Li, and Dong Guo
Atmos. Chem. Phys., 20, 8627–8639, https://doi.org/10.5194/acp-20-8627-2020, https://doi.org/10.5194/acp-20-8627-2020, 2020
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The Tibetan Plateau (TP) exerts important thermal and dynamical effects on atmospheric circulation, climate change as well as the ozone distribution. In this study, we use updated observations and model simulations to investigate the ozone trends and variations over the TP. Wintertime TP ozone variations are largely controlled by tropical to high-latitude transport processes, whereas summertime concentrations are a combined effect of photochemical decay and tropical processes.
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.
Daniele Visioni, Giovanni Pitari, Vincenzo Rizi, Marco Iarlori, Irene Cionni, Ilaria Quaglia, Hideharu Akiyoshi, Slimane Bekki, Neal Butchart, Martin Chipperfield, Makoto Deushi, Sandip S. Dhomse, Rolando Garcia, Patrick Joeckel, Douglas Kinnison, Jean-François Lamarque, Marion Marchand, Martine Michou, Olaf Morgenstern, Tatsuya Nagashima, Fiona M. O'Connor, Luke D. Oman, David Plummer, Eugene Rozanov, David Saint-Martin, Robyn Schofield, John Scinocca, Andrea Stenke, Kane Stone, Kengo Sudo, Taichu Y. Tanaka, Simone Tilmes, Holger Tost, Yousuke Yamashita, and Guang Zeng
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-525, https://doi.org/10.5194/acp-2020-525, 2020
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In this work we analyse the trend in ozone profiles taken at L'Aquila (Italy, 42.4° N) for seventeen years, between 2000 and 2016 and compare them against already available measured ozone trends. We try to understand and explain the observed trends at various heights in light of the simulations from seventeen different model, highlighting the contribution of changes in circulation and chemical ozone loss during this time period.
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.
James Keeble, N. Luke Abraham, Alexander T. Archibald, Martyn P. Chipperfield, Sandip Dhomse, Paul T. Griffiths, and John A. Pyle
Atmos. Chem. Phys., 20, 7153–7166, https://doi.org/10.5194/acp-20-7153-2020, https://doi.org/10.5194/acp-20-7153-2020, 2020
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The Montreal Protocol was agreed in 1987 to limit and then stop the production of man-made CFCs, which destroy stratospheric ozone. As a result, the atmospheric abundances of CFCs are now declining in the atmosphere. However, the atmospheric abundance of CFC-11 is not declining as expected under complete compliance with the Montreal Protocol. Using the UM-UKCA chemistry–climate model, we explore the impact of future unregulated production of CFC-11 on ozone recovery.
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.
Andreas Chrysanthou, Amanda C. Maycock, and Martyn P. Chipperfield
Weather Clim. Dynam., 1, 155–174, https://doi.org/10.5194/wcd-1-155-2020, https://doi.org/10.5194/wcd-1-155-2020, 2020
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We perform 50-year-long time-slice experiments using the Met Office HadGEM3 global climate model in order to decompose the Brewer–Dobson circulation (BDC) response to an abrupt quadrupling of CO2 in three distinct components, (a) the rapid adjustment, associated with CO2 radiative effects; (b) a global uniform sea surface temperature warming; and (c) sea surface temperature patterns. This demonstrates a potential for fast and slow timescales of the response of the BDC to greenhouse gas forcing.
Didier G. Leibovici, Shaun Quegan, Edward Comyn-Platt, Garry Hayman, Maria Val Martin, Mathieu Guimberteau, Arsène Druel, Dan Zhu, and Philippe Ciais
Biogeosciences, 17, 1821–1844, https://doi.org/10.5194/bg-17-1821-2020, https://doi.org/10.5194/bg-17-1821-2020, 2020
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Analysing the impact of environmental changes due to climate change, e.g. geographical spread of climate-sensitive infections (CSIs) and agriculture crop modelling, may require land surface modelling (LSM) to predict future land surface conditions. There are multiple LSMs to choose from. The paper proposes a multivariate spatio-temporal data science method to understand the inherent uncertainties in four LSMs and the variations between them in Nordic areas for the net primary production.
Clara Orbe, David A. Plummer, Darryn W. Waugh, Huang Yang, Patrick Jöckel, Douglas E. Kinnison, Beatrice Josse, Virginie Marecal, Makoto Deushi, Nathan Luke Abraham, Alexander T. Archibald, Martyn P. Chipperfield, Sandip Dhomse, Wuhu Feng, and Slimane Bekki
Atmos. Chem. Phys., 20, 3809–3840, https://doi.org/10.5194/acp-20-3809-2020, https://doi.org/10.5194/acp-20-3809-2020, 2020
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Atmospheric composition is strongly influenced by global-scale winds that are not always properly simulated in computer models. A common approach to correct for this bias is to relax or
nudgeto the observed winds. Here we systematically evaluate how well this technique performs across a large suite of chemistry–climate models in terms of its ability to reproduce key aspects of both the tropospheric and stratospheric circulations.
Alexander T. Archibald, Fiona M. O'Connor, Nathan Luke Abraham, Scott Archer-Nicholls, Martyn P. Chipperfield, Mohit Dalvi, Gerd A. Folberth, Fraser Dennison, Sandip S. Dhomse, Paul T. Griffiths, Catherine Hardacre, Alan J. Hewitt, Richard S. Hill, Colin E. Johnson, James Keeble, Marcus O. Köhler, Olaf Morgenstern, Jane P. Mulcahy, Carlos Ordóñez, Richard J. Pope, Steven T. Rumbold, Maria R. Russo, Nicholas H. Savage, Alistair Sellar, Marc Stringer, Steven T. Turnock, Oliver Wild, and Guang Zeng
Geosci. Model Dev., 13, 1223–1266, https://doi.org/10.5194/gmd-13-1223-2020, https://doi.org/10.5194/gmd-13-1223-2020, 2020
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Here we present a description and evaluation of the UKCA stratosphere–troposphere chemistry scheme (StratTrop vn 1.0) implemented in the UK Earth System Model (UKESM1). UKCA StratTrop represents a substantial step forward compared to previous versions of UKCA. We show here that it is fully suited to the challenges of representing interactions in a coupled Earth system model and identify key areas and components for future development that will make it even better in the future.
Jian He, Vaishali Naik, Larry W. Horowitz, Ed Dlugokencky, and Kirk Thoning
Atmos. Chem. Phys., 20, 805–827, https://doi.org/10.5194/acp-20-805-2020, https://doi.org/10.5194/acp-20-805-2020, 2020
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In this work, methane representation in AM4.1 is improved by optimizing CH4 emissions to match surface observations. We find increases in CH4 sources balanced by increases in sinks lead to CH4 stabilization during 1999–2006, and anthropogenic sources (e.g., agriculture, energy, and waste) are more likely major contributors to the renewed growth after 2006. Increases in CH4 emissions and decreases in OH levels during 2008–2015 prolong CH4 lifetime and amplify methane response to emission changes.
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.
Yuanhong Zhao, Marielle Saunois, Philippe Bousquet, Xin Lin, Antoine Berchet, Michaela I. Hegglin, Josep G. Canadell, Robert B. Jackson, Didier A. Hauglustaine, Sophie Szopa, Ann R. Stavert, Nathan Luke Abraham, Alex T. Archibald, Slimane Bekki, Makoto Deushi, Patrick Jöckel, Béatrice Josse, Douglas Kinnison, Ole Kirner, Virginie Marécal, Fiona M. O'Connor, David A. Plummer, Laura E. Revell, Eugene Rozanov, Andrea Stenke, Sarah Strode, Simone Tilmes, Edward J. Dlugokencky, and Bo Zheng
Atmos. Chem. Phys., 19, 13701–13723, https://doi.org/10.5194/acp-19-13701-2019, https://doi.org/10.5194/acp-19-13701-2019, 2019
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The role of hydroxyl radical changes in methane trends is debated, hindering our understanding of the methane cycle. This study quantifies how uncertainties in the hydroxyl radical may influence methane abundance in the atmosphere based on the inter-model comparison of hydroxyl radical fields and model simulations of CH4 abundance with different hydroxyl radical scenarios during 2000–2016. We show that hydroxyl radical changes could contribute up to 54 % of model-simulated methane biases.
Susan S. Kulawik, Sean Crowell, David Baker, Junjie Liu, Kathryn McKain, Colm Sweeney, Sebastien C. Biraud, Steve Wofsy, Christopher W. O'Dell, Paul O. Wennberg, Debra Wunch, Coleen M. Roehl, Nicholas M. Deutscher, Matthäus Kiel, David W. T. Griffith, Voltaire A. Velazco, Justus Notholt, Thorsten Warneke, Christof Petri, Martine De Mazière, Mahesh K. Sha, Ralf Sussmann, Markus Rettinger, Dave F. Pollard, Isamu Morino, Osamu Uchino, Frank Hase, Dietrich G. Feist, Sébastien Roche, Kimberly Strong, Rigel Kivi, Laura Iraci, Kei Shiomi, Manvendra K. Dubey, Eliezer Sepulveda, Omaira Elena Garcia Rodriguez, Yao Té, Pascal Jeseck, Pauli Heikkinen, Edward J. Dlugokencky, Michael R. Gunson, Annmarie Eldering, David Crisp, Brendan Fisher, and Gregory B. Osterman
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2019-257, https://doi.org/10.5194/amt-2019-257, 2019
Publication in AMT not foreseen
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This paper provides a benchmark of OCO-2 v8 and ACOS-GOSAT v7.3 XCO2 and lowermost tropospheric (LMT) errors. The paper focuses on the systematic errors and subtracts out validation, co-location, and random errors, looks at the correlation scale-length (spatially and temporally) of systematic errors, finding that the scale lengths are similar to bias correction scale-lengths. The assimilates of the bias correction term is used to place an error on fluxes estimates.
Maxime Prignon, Simon Chabrillat, Daniele Minganti, Simon O'Doherty, Christian Servais, Gabriele Stiller, Geoffrey C. Toon, Martin K. Vollmer, and Emmanuel Mahieu
Atmos. Chem. Phys., 19, 12309–12324, https://doi.org/10.5194/acp-19-12309-2019, https://doi.org/10.5194/acp-19-12309-2019, 2019
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Hydrochlorofluorocarbons (HCFCs) are the first, but temporary, substitution products for the strong ozone-depleting chlorofluorocarbons (CFCs). In this work, we present and validate an improved method to retrieve the most abundant HCFC in the atmosphere, allowing its evolution to be monitored independently in the troposphere and stratosphere. These kinds of contributions are fundamental for scrutinizing the fulfilment of the Montreal Protocol on Substances that Deplete the Ozone Layer.
Andreas Chrysanthou, Amanda C. Maycock, Martyn P. Chipperfield, Sandip Dhomse, Hella Garny, Douglas Kinnison, Hideharu Akiyoshi, Makoto Deushi, Rolando R. Garcia, Patrick Jöckel, Oliver Kirner, Giovanni Pitari, David A. Plummer, Laura Revell, Eugene Rozanov, Andrea Stenke, Taichu Y. Tanaka, Daniele Visioni, and Yousuke Yamashita
Atmos. Chem. Phys., 19, 11559–11586, https://doi.org/10.5194/acp-19-11559-2019, https://doi.org/10.5194/acp-19-11559-2019, 2019
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We perform the first multi-model comparison of the impact of nudged meteorology on the stratospheric residual circulation (RC) in chemistry–climate models. Nudging meteorology does not constrain the mean strength of RC compared to free-running simulations, and despite the lack of agreement in the mean circulation, nudging tightly constrains the inter-annual variability in the tropical upward mass flux in the lower stratosphere. In summary, nudging strongly affects the representation of RC.
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.
Kévin Lamy, Thierry Portafaix, Béatrice Josse, Colette Brogniez, Sophie Godin-Beekmann, Hassan Bencherif, Laura Revell, Hideharu Akiyoshi, Slimane Bekki, Michaela I. Hegglin, Patrick Jöckel, Oliver Kirner, Ben Liley, Virginie Marecal, Olaf Morgenstern, Andrea Stenke, Guang Zeng, N. Luke Abraham, Alexander T. Archibald, Neil Butchart, Martyn P. Chipperfield, Glauco Di Genova, Makoto Deushi, Sandip S. Dhomse, Rong-Ming Hu, Douglas Kinnison, Michael Kotkamp, Richard McKenzie, Martine Michou, Fiona M. O'Connor, Luke D. Oman, Giovanni Pitari, David A. Plummer, John A. Pyle, Eugene Rozanov, David Saint-Martin, Kengo Sudo, Taichu Y. Tanaka, Daniele Visioni, and Kohei Yoshida
Atmos. Chem. Phys., 19, 10087–10110, https://doi.org/10.5194/acp-19-10087-2019, https://doi.org/10.5194/acp-19-10087-2019, 2019
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In this study, we simulate the ultraviolet radiation evolution during the 21st century on Earth's surface using the output from several numerical models which participated in the Chemistry-Climate Model Initiative. We present four possible futures which depend on greenhouse gases emissions. The role of ozone-depleting substances, greenhouse gases and aerosols are investigated. Our results emphasize the important role of aerosols for future ultraviolet radiation in the Northern Hemisphere.
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.
Matthew J. Rowlinson, Alexandru Rap, Stephen R. Arnold, Richard J. Pope, Martyn P. Chipperfield, Joe McNorton, Piers Forster, Hamish Gordon, Kirsty J. Pringle, Wuhu Feng, Brian J. Kerridge, Barry L. Latter, and Richard Siddans
Atmos. Chem. Phys., 19, 8669–8686, https://doi.org/10.5194/acp-19-8669-2019, https://doi.org/10.5194/acp-19-8669-2019, 2019
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Wildfires and meteorology have a substantial effect on atmospheric concentrations of greenhouse gases such as methane and ozone. During the 1997 El Niño event, unusually large fire emissions indirectly increased global methane through carbon monoxide emission, which decreased the oxidation capacity of the atmosphere. There were also large regional changes to tropospheric ozone concentrations, but contrasting effects of fire and meteorology resulted in a small change to global radiative forcing.
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.
Evgenia Galytska, Alexey Rozanov, Martyn P. Chipperfield, Sandip. S. Dhomse, Mark Weber, Carlo Arosio, Wuhu Feng, and John P. Burrows
Atmos. Chem. Phys., 19, 767–783, https://doi.org/10.5194/acp-19-767-2019, https://doi.org/10.5194/acp-19-767-2019, 2019
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In this study we analysed ozone changes in the tropical mid-stratosphere as observed by the SCIAMACHY instrument during 2004–2012. We used simulations from TOMCAT model with different chemical and dynamical forcings to reveal primary causes of ozone changes. We also considered measured NO2 and modelled NOx, NOx, and N2O data. With modelled AoA data we identified seasonal changes in the upwelling speed and explained how those changes affect N2O chemistry which leads to observed ozone changes.
Debora Griffin, Kaley A. Walker, Ingo Wohltmann, Sandip S. Dhomse, Markus Rex, Martyn P. Chipperfield, Wuhu Feng, Gloria L. Manney, Jane Liu, and David Tarasick
Atmos. Chem. Phys., 19, 577–601, https://doi.org/10.5194/acp-19-577-2019, https://doi.org/10.5194/acp-19-577-2019, 2019
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Ozone in the stratosphere is important to protect the Earth from UV radiation. Using measurements taken by the Atmospheric Chemistry Experiment satellite between 2005 and 2013, we examine different methods to calculate the ozone loss in the high Arctic and establish the altitude at which most of the ozone is destroyed. Our results show that the different methods agree within the uncertainties. Recommendations are made on which methods are most appropriate to use.
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.
Joe McNorton, Chris Wilson, Manuel Gloor, Rob J. Parker, Hartmut Boesch, Wuhu Feng, Ryan Hossaini, and Martyn P. Chipperfield
Atmos. Chem. Phys., 18, 18149–18168, https://doi.org/10.5194/acp-18-18149-2018, https://doi.org/10.5194/acp-18-18149-2018, 2018
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Since 2007 atmospheric methane (CH4) has been unexpectedly increasing following a 6-year hiatus. We have used an atmospheric model to attribute regional sources and global sinks of CH4 using observations for the 2003–2015 period. Model results show the renewed growth is best explained by decreased atmospheric removal, decreased biomass burning emissions, and an increased energy sector (mainly from Africa–Middle East and Southern Asia–Oceania) and wetland emissions (mainly from northern Eurasia).
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.
Christine D. Groot Zwaaftink, Stephan Henne, Rona L. Thompson, Edward J. Dlugokencky, Toshinobu Machida, Jean-Daniel Paris, Motoki Sasakawa, Arjo Segers, Colm Sweeney, and Andreas Stohl
Geosci. Model Dev., 11, 4469–4487, https://doi.org/10.5194/gmd-11-4469-2018, https://doi.org/10.5194/gmd-11-4469-2018, 2018
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A Lagrangian particle dispersion model is used to simulate global fields of methane, constrained by observations through nudging. We show that this rather simple and computationally inexpensive method can give results similar to or as good as a computationally expensive Eulerian chemistry transport model with a data assimilation scheme. The three-dimensional methane fields are of interest to applications such as inverse modelling and satellite retrievals.
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.
Birgit Hassler, Stefanie Kremser, Greg E. Bodeker, Jared Lewis, Kage Nesbit, Sean M. Davis, Martyn P. Chipperfield, Sandip S. Dhomse, and Martin Dameris
Earth Syst. Sci. Data, 10, 1473–1490, https://doi.org/10.5194/essd-10-1473-2018, https://doi.org/10.5194/essd-10-1473-2018, 2018
Maarten Krol, Marco de Bruine, Lars Killaars, Huug Ouwersloot, Andrea Pozzer, Yi Yin, Frederic Chevallier, Philippe Bousquet, Prabir Patra, Dmitry Belikov, Shamil Maksyutov, Sandip Dhomse, Wuhu Feng, and Martyn P. Chipperfield
Geosci. Model Dev., 11, 3109–3130, https://doi.org/10.5194/gmd-11-3109-2018, https://doi.org/10.5194/gmd-11-3109-2018, 2018
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The TransCom inter-comparison project regularly carries out studies to quantify errors in simulated atmospheric transport. This paper presents the first results of an age of air (AoA) inter-comparison of six global transport models. Following a protocol, six models simulated five tracers from which atmospheric transport times can easily be deduced. Results highlight that inter-model differences associated with atmospheric transport are still large and require further analysis.
Jens-Uwe Grooß, Rolf Müller, Reinhold Spang, Ines Tritscher, Tobias Wegner, Martyn P. Chipperfield, Wuhu Feng, Douglas E. Kinnison, and Sasha Madronich
Atmos. Chem. Phys., 18, 8647–8666, https://doi.org/10.5194/acp-18-8647-2018, https://doi.org/10.5194/acp-18-8647-2018, 2018
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We investigate a discrepancy between model simulations and observations of HCl in the dark polar stratosphere. In early winter, the less-well-studied period of the onset of chlorine activation, observations show a much faster depletion of HCl than simulations of three models. This points to some unknown process that is currently not represented in the models. Various hypotheses for potential causes are investigated that partly reduce the discrepancy. The impact on polar ozone depletion is low.
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.
Richard J. Pope, Martyn P. Chipperfield, Stephen R. Arnold, Norbert Glatthor, Wuhu Feng, Sandip S. Dhomse, Brian J. Kerridge, Barry G. Latter, and Richard Siddans
Atmos. Chem. Phys., 18, 8389–8408, https://doi.org/10.5194/acp-18-8389-2018, https://doi.org/10.5194/acp-18-8389-2018, 2018
Sandip S. Dhomse, Douglas Kinnison, Martyn P. Chipperfield, Ross J. Salawitch, Irene Cionni, Michaela I. Hegglin, N. Luke Abraham, Hideharu Akiyoshi, Alex T. Archibald, Ewa M. Bednarz, Slimane Bekki, Peter Braesicke, Neal Butchart, Martin Dameris, Makoto Deushi, Stacey Frith, Steven C. Hardiman, Birgit Hassler, Larry W. Horowitz, Rong-Ming Hu, Patrick Jöckel, Beatrice Josse, Oliver Kirner, Stefanie Kremser, Ulrike Langematz, Jared Lewis, Marion Marchand, Meiyun Lin, Eva Mancini, Virginie Marécal, Martine Michou, Olaf Morgenstern, Fiona M. O'Connor, Luke Oman, Giovanni Pitari, David A. Plummer, John A. Pyle, Laura E. Revell, Eugene Rozanov, Robyn Schofield, Andrea Stenke, Kane Stone, Kengo Sudo, Simone Tilmes, Daniele Visioni, Yousuke Yamashita, and Guang Zeng
Atmos. Chem. Phys., 18, 8409–8438, https://doi.org/10.5194/acp-18-8409-2018, https://doi.org/10.5194/acp-18-8409-2018, 2018
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We analyse simulations from the Chemistry-Climate Model Initiative (CCMI) to estimate the return dates of the stratospheric ozone layer from depletion by anthropogenic chlorine and bromine. The simulations from 20 models project that global column ozone will return to 1980 values in 2047 (uncertainty range 2042–2052). Return dates in other regions vary depending on factors related to climate change and importance of chlorine and bromine. Column ozone in the tropics may continue to decline.
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.
Andreas Engel, Harald Bönisch, Jennifer Ostermöller, Martyn P. Chipperfield, Sandip Dhomse, and Patrick Jöckel
Atmos. Chem. Phys., 18, 601–619, https://doi.org/10.5194/acp-18-601-2018, https://doi.org/10.5194/acp-18-601-2018, 2018
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We present a new method to derive equivalent effective stratospheric chlorine (EESC), which is based on an improved formulation of the propagation of trends of species with chemical loss from the troposphere to the stratosphere. EESC calculated with the new method shows much better agreement with model-derived ESC. Based on this new formulation, we expect the halogen impact on midlatitude stratospheric ozone to return to 1980 values about 10 years later, then using the current formulation.
Daniel R. Moon, Giorgio S. Taverna, Clara Anduix-Canto, Trevor Ingham, Martyn P. Chipperfield, Paul W. Seakins, Maria-Teresa Baeza-Romero, and Dwayne E. Heard
Atmos. Chem. Phys., 18, 327–338, https://doi.org/10.5194/acp-18-327-2018, https://doi.org/10.5194/acp-18-327-2018, 2018
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One geoengineering mitigation strategy for global temperature rises is to inject particles into the stratosphere to scatter solar radiation back to space. However, the injection of such particles must not perturb ozone. We measured the rate of uptake of HO2 radicals, an important stratospheric intermediate, onto TiO2 particles. Using the atmospheric model TOMCAT, we showed that surface reactions between HO2 and TiO2 would have a negligible effect on stratospheric concentrations of HO2 and ozone.
Xin Lan, Pieter Tans, Colm Sweeney, Arlyn Andrews, Andrew Jacobson, Molly Crotwell, Edward Dlugokencky, Jonathan Kofler, Patricia Lang, Kirk Thoning, and Sonja Wolter
Atmos. Chem. Phys., 17, 15151–15165, https://doi.org/10.5194/acp-17-15151-2017, https://doi.org/10.5194/acp-17-15151-2017, 2017
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We analyze spatial patterns of column CO2 over North America using well-calibrated aircraft and tall tower measurements. We find that the long-term averaged spatial gradients of column CO2 across North America show a smooth pattern that mainly reflects the large-scale circulation. Our results can serve as a good reference for evaluating current and future column CO2 retrievals from both ground and satellite platforms.
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.
Sarah A. Monks, Stephen R. Arnold, Michael J. Hollaway, Richard J. Pope, Chris Wilson, Wuhu Feng, Kathryn M. Emmerson, Brian J. Kerridge, Barry L. Latter, Georgina M. Miles, Richard Siddans, and Martyn P. Chipperfield
Geosci. Model Dev., 10, 3025–3057, https://doi.org/10.5194/gmd-10-3025-2017, https://doi.org/10.5194/gmd-10-3025-2017, 2017
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The TOMCAT chemical transport model has been updated with the chemical degradation of ethene, propene, toluene, butane and monoterpenes. The tropospheric chemical mechanism is documented and the model is evaluated against surface, balloon, aircraft and satellite data. The model is generally able to capture the main spatial and seasonal features of carbon monoxide, ozone, volatile organic compounds and reactive nitrogen. However,
some model biases are found that require further investigation.
Chris Huntingford, Hui Yang, Anna Harper, Peter M. Cox, Nicola Gedney, Eleanor J. Burke, Jason A. Lowe, Garry Hayman, William J. Collins, Stephen M. Smith, and Edward Comyn-Platt
Earth Syst. Dynam., 8, 617–626, https://doi.org/10.5194/esd-8-617-2017, https://doi.org/10.5194/esd-8-617-2017, 2017
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Recent UNFCCC climate meetings have placed much emphasis on constraining global warming to remain below 2 °C. The 2015 Paris meeting went further and gave an aspiration to fulfil a 1.5 °C threshold. We provide a flexible set of algebraic global temperature profiles that stabilise to either target. This will potentially allow the climate research community to estimate local climatic implications for these temperature profiles, along with emissions trajectories to fulfil them.
Thibaud Thonat, Marielle Saunois, Philippe Bousquet, Isabelle Pison, Zeli Tan, Qianlai Zhuang, Patrick M. Crill, Brett F. Thornton, David Bastviken, Ed J. Dlugokencky, Nikita Zimov, Tuomas Laurila, Juha Hatakka, Ove Hermansen, and Doug E. J. Worthy
Atmos. Chem. Phys., 17, 8371–8394, https://doi.org/10.5194/acp-17-8371-2017, https://doi.org/10.5194/acp-17-8371-2017, 2017
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Atmospheric methane simulations in the Arctic have been made for 2012 and compared to continuous observations at six measurement sites. All methane sources significantly affect the measurements at all stations, at least at the synoptic scale, except for biomass burning. An appropriate modelling framework combined with continuous observations of atmospheric methane enables us to gain knowledge on regional methane sources, including those which are usually poorly represented, such as freshwater.
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.
Wenshou Tian, Yuanpu Li, Fei Xie, Jiankai Zhang, Martyn P. Chipperfield, Wuhu Feng, Yongyun Hu, Sen Zhao, Xin Zhou, Yun Yang, and Xuan Ma
Atmos. Chem. Phys., 17, 6705–6722, https://doi.org/10.5194/acp-17-6705-2017, https://doi.org/10.5194/acp-17-6705-2017, 2017
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Although the principal mechanisms responsible for the formation of the Antarctic ozone hole are well understood, the factors or processes that generate interannual variations in ozone levels in the southern high-latitude stratosphere remain under debate. This study finds that the SST variations across the East Asian marginal seas (5° S–35° N, 100–140° E) could modulate the southern high-latitude stratospheric ozone interannual changes.
Shreeya Verma, Julia Marshall, Mark Parrington, Anna Agustí-Panareda, Sebastien Massart, Martyn P. Chipperfield, Christopher Wilson, and Christoph Gerbig
Atmos. Chem. Phys., 17, 6663–6678, https://doi.org/10.5194/acp-17-6663-2017, https://doi.org/10.5194/acp-17-6663-2017, 2017
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Aircraft profiles are a useful reference for validation of satellite-based column-averaged dry air mole fraction data. However, these are available only up to about 9–13 km altitude and therefore need to be extended synthetically into the stratosphere using other sources. In this study, we analyse three different data sources that are available for extension of CH4 profiles by comparing the error introduced by each into the total column and provide recommendations regarding the best approach.
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.
Markella Prokopiou, Patricia Martinerie, Célia J. Sapart, Emmanuel Witrant, Guillaume Monteil, Kentaro Ishijima, Sophie Bernard, Jan Kaiser, Ingeborg Levin, Thomas Blunier, David Etheridge, Ed Dlugokencky, Roderik S. W. van de Wal, and Thomas Röckmann
Atmos. Chem. Phys., 17, 4539–4564, https://doi.org/10.5194/acp-17-4539-2017, https://doi.org/10.5194/acp-17-4539-2017, 2017
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Nitrous oxide is the third most important anthropogenic greenhouse gas with an increasing mole fraction. To understand its natural and anthropogenic sources
we employ isotope measurements. Results show that while the N2O mole fraction increases, its heavy isotope content decreases. The isotopic changes observed underline the dominance of agricultural emissions especially at the early part of the record, whereas in the later decades the contribution from other anthropogenic sources increases.
Aki Tsuruta, Tuula Aalto, Leif Backman, Janne Hakkarainen, Ingrid T. van der Laan-Luijkx, Maarten C. Krol, Renato Spahni, Sander Houweling, Marko Laine, Ed Dlugokencky, Angel J. Gomez-Pelaez, Marcel van der Schoot, Ray Langenfelds, Raymond Ellul, Jgor Arduini, Francesco Apadula, Christoph Gerbig, Dietrich G. Feist, Rigel Kivi, Yukio Yoshida, and Wouter Peters
Geosci. Model Dev., 10, 1261–1289, https://doi.org/10.5194/gmd-10-1261-2017, https://doi.org/10.5194/gmd-10-1261-2017, 2017
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In this study, we found that the average global methane emission for 2000–2012, estimated by the CTE-CH4 model, was 516±51 Tg CH4 yr-1, and the estimates for 2007–2012 were 4 % larger than for 2000–2006. The model estimates are sensitive to inputs and setups, but according to sensitivity tests the study suggests that the increase in atmospheric methane concentrations during 21st century was due to an increase in emissions from the 35S-EQ latitudinal bands.
Jochen Stutz, Bodo Werner, Max Spolaor, Lisa Scalone, James Festa, Catalina Tsai, Ross Cheung, Santo F. Colosimo, Ugo Tricoli, Rasmus Raecke, Ryan Hossaini, Martyn P. Chipperfield, Wuhu Feng, Ru-Shan Gao, Eric J. Hintsa, James W. Elkins, Fred L. Moore, Bruce Daube, Jasna Pittman, Steven Wofsy, and Klaus Pfeilsticker
Atmos. Meas. Tech., 10, 1017–1042, https://doi.org/10.5194/amt-10-1017-2017, https://doi.org/10.5194/amt-10-1017-2017, 2017
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A new limb-scanning Differential Optical Absorption Spectroscopy (DOAS) instrument was developed for NASA’s Global Hawk unmanned aerial system during the Airborne Tropical TRopopause EXperiment to study trace gases in the tropical tropopause layer. A new technique that uses in situ and DOAS O3 observations together with radiative transfer calculations allows the retrieval of mixing ratios from the slant column densities of BrO and NO2 at high accuracies of 0.5 ppt and 15 ppt, respectively.
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.
Olaf Morgenstern, Michaela I. Hegglin, Eugene Rozanov, Fiona M. O'Connor, N. Luke Abraham, Hideharu Akiyoshi, Alexander T. Archibald, Slimane Bekki, Neal Butchart, Martyn P. Chipperfield, Makoto Deushi, Sandip S. Dhomse, Rolando R. Garcia, Steven C. Hardiman, Larry W. Horowitz, Patrick Jöckel, Beatrice Josse, Douglas Kinnison, Meiyun Lin, Eva Mancini, Michael E. Manyin, Marion Marchand, Virginie Marécal, Martine Michou, Luke D. Oman, Giovanni Pitari, David A. Plummer, Laura E. Revell, David Saint-Martin, Robyn Schofield, Andrea Stenke, Kane Stone, Kengo Sudo, Taichu Y. Tanaka, Simone Tilmes, Yousuke Yamashita, Kohei Yoshida, and Guang Zeng
Geosci. Model Dev., 10, 639–671, https://doi.org/10.5194/gmd-10-639-2017, https://doi.org/10.5194/gmd-10-639-2017, 2017
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We present a review of the make-up of 20 models participating in the Chemistry–Climate Model Initiative (CCMI). In comparison to earlier such activities, most of these models comprise a whole-atmosphere chemistry, and several of them include an interactive ocean module. This makes them suitable for studying the interactions of tropospheric air quality, stratospheric ozone, and climate. The paper lays the foundation for other studies using the CCMI simulations for scientific analysis.
Bodo Werner, Jochen Stutz, Max Spolaor, Lisa Scalone, Rasmus Raecke, James Festa, Santo Fedele Colosimo, Ross Cheung, Catalina Tsai, Ryan Hossaini, Martyn P. Chipperfield, Giorgio S. Taverna, Wuhu Feng, James W. Elkins, David W. Fahey, Ru-Shan Gao, Erik J. Hintsa, Troy D. Thornberry, Free Lee Moore, Maria A. Navarro, Elliot Atlas, Bruce C. Daube, Jasna Pittman, Steve Wofsy, and Klaus Pfeilsticker
Atmos. Chem. Phys., 17, 1161–1186, https://doi.org/10.5194/acp-17-1161-2017, https://doi.org/10.5194/acp-17-1161-2017, 2017
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The paper reports on inorganic and organic bromine measured in the tropical tropopause layer (TTL) over the eastern Pacific in early 2013. Bryinorg is found to increase from a mean of 2.63 ± 1.04 ppt for θ in the range of 350–360 K to 5.11 ± 1.57 ppt for θ=390 ± 400 K, whereas in the subtropical lower stratosphere, it reaches 7.66 ± 2.95 ppt for θ in the range of 390–400 K. Within the TTL, total bromine is found to range from 20.3 ppt to 22.3 ppt.
Tamás Kovács, Wuhu Feng, Anna Totterdill, John M. C. Plane, Sandip Dhomse, Juan Carlos Gómez-Martín, Gabriele P. Stiller, Florian J. Haenel, Christopher Smith, Piers M. Forster, Rolando R. García, Daniel R. Marsh, and Martyn P. Chipperfield
Atmos. Chem. Phys., 17, 883–898, https://doi.org/10.5194/acp-17-883-2017, https://doi.org/10.5194/acp-17-883-2017, 2017
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Sulfur hexafluoride (SF6) is a very potent greenhouse gas, which is present in the atmosphere only through its industrial use, for example as an electrical insulator. To estimate accurately the impact of SF6 emissions on climate we need to know how long it persists in the atmosphere before being removed. Previous estimates of the SF6 lifetime indicate a large degree of uncertainty. Here we use a detailed atmospheric model to calculate a current best estimate of the SF6 lifetime.
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.
Richard J. Pope, Nigel A. D. Richards, Martyn P. Chipperfield, David P. Moore, Sarah A. Monks, Stephen R. Arnold, Norbert Glatthor, Michael Kiefer, Tom J. Breider, Jeremy J. Harrison, John J. Remedios, Carsten Warneke, James M. Roberts, Glenn S. Diskin, Lewis G. Huey, Armin Wisthaler, Eric C. Apel, Peter F. Bernath, and Wuhu Feng
Atmos. Chem. Phys., 16, 13541–13559, https://doi.org/10.5194/acp-16-13541-2016, https://doi.org/10.5194/acp-16-13541-2016, 2016
Florian Obersteiner, Harald Bönisch, Timo Keber, Simon O'Doherty, and Andreas Engel
Atmos. Meas. Tech., 9, 5265–5279, https://doi.org/10.5194/amt-9-5265-2016, https://doi.org/10.5194/amt-9-5265-2016, 2016
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The analysis of trace gases in ambient air requires a preconcentration technique, in many cases to make the species of interest detectable and quantifiable. In this paper, such a preconcentration set-up is presented. Target species are trapped on adsorptive material cooled by a Stirling cooler which allows for a very low adsorption temperature but only requires electrical power. A simple and lightweight mechanical design guarantees very good suitability for remote-site field operation.
Francesco Graziosi, Jgor Arduini, Paolo Bonasoni, Francesco Furlani, Umberto Giostra, Alistair J. Manning, Archie McCulloch, Simon O'Doherty, Peter G. Simmonds, Stefan Reimann, Martin K. Vollmer, and Michela Maione
Atmos. Chem. Phys., 16, 12849–12859, https://doi.org/10.5194/acp-16-12849-2016, https://doi.org/10.5194/acp-16-12849-2016, 2016
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Carbon tetrachloride is an ozone-depleting greenhouse gas banned under the Montreal Protocol. Measurements of atmospheric levels combined with global transport models indicate that it is still being emitted, in contrast to what is reported. In order to help solve the "mystery of carbon tetrachloride", we estimated European emissions during 2006–2014 using atmospheric observations and models. We identified emission hot spots and showed inconsistencies in national emission declarations.
Zeli Tan, Qianlai Zhuang, Daven K. Henze, Christian Frankenberg, Ed Dlugokencky, Colm Sweeney, Alexander J. Turner, Motoki Sasakawa, and Toshinobu Machida
Atmos. Chem. Phys., 16, 12649–12666, https://doi.org/10.5194/acp-16-12649-2016, https://doi.org/10.5194/acp-16-12649-2016, 2016
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Methane emissions from the pan-Arctic could be important in understanding the global carbon cycle but are still poorly constrained to date. This study demonstrated that satellite retrievals can be used to reduce the uncertainty of the estimates of these emissions. We also provided additional evidence for the existence of large methane emissions from pan-Arctic lakes in the Siberian yedoma permafrost region. We found that biogeochemical models should be improved for better estimates.
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.
Anna Totterdill, Tamás Kovács, Wuhu Feng, Sandip Dhomse, Christopher J. Smith, Juan Carlos Gómez-Martín, Martyn P. Chipperfield, Piers M. Forster, and John M. C. Plane
Atmos. Chem. Phys., 16, 11451–11463, https://doi.org/10.5194/acp-16-11451-2016, https://doi.org/10.5194/acp-16-11451-2016, 2016
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In this study we have experimentally determined the infrared absorption cross sections of NF3 and CFC-115, calculated the radiative forcing and efficiency using two radiative transfer models and identified the effect of clouds and stratospheric adjustment. We have also determined their atmospheric lifetimes using the Whole Atmosphere Community Climate Model.
Tamás Kovács, John M. C. Plane, Wuhu Feng, Tibor Nagy, Martyn P. Chipperfield, Pekka T. Verronen, Monika E. Andersson, David A. Newnham, Mark A. Clilverd, and Daniel R. Marsh
Geosci. Model Dev., 9, 3123–3136, https://doi.org/10.5194/gmd-9-3123-2016, https://doi.org/10.5194/gmd-9-3123-2016, 2016
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This study was completed on D-region atmospheric model development. The sophisticated 3-D Whole Atmosphere Community Climate Model (WACCM) and the 1-D Sodynkalä Ion and Neutral Chemistry Model (SIC) were combined in order to provide a detailed, accurate model (WACCM-SIC) that considers the processes taking place in solar proton events. The original SIC model was reduced by mechanism reduction, which provided an accurate sub-mechanism (rSIC, WACCM-rSIC) of the original model.
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.
Congsheng Fu, Xuhui Lee, Timothy J. Griffis, Edward J. Dlugokencky, and Arlyn E. Andrews
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2016-761, https://doi.org/10.5194/acp-2016-761, 2016
Revised manuscript not accepted
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To the best of our knowledge, no modeling studies have been published on the relationship between the spatial characteristics of agricultural N2O emissions and the atmospheric N2O mixing ratio at the regional scale. To fill this gap, we proposed a simple inverse analysis method based on tower measurements and an Eulerian model. According to our study, the N2O emissions from the U. S. Corn Belt is clearly estimated by IPCC, and such underestimate is not dependent on tower measurement location.
Jeremy J. Harrison, Martyn P. Chipperfield, Christopher D. Boone, Sandip S. Dhomse, Peter F. Bernath, Lucien Froidevaux, John Anderson, and James Russell III
Atmos. Chem. Phys., 16, 10501–10519, https://doi.org/10.5194/acp-16-10501-2016, https://doi.org/10.5194/acp-16-10501-2016, 2016
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HF, the dominant stratospheric fluorine reservoir, results from the atmospheric degradation of anthropogenic species such as CFCs, HCFCs, and HFCs. All are strong greenhouse gases, and CFCs and HCFCs deplete stratospheric ozone.
We report the comparison of HF global distributions and trends measured by the ACE-FTS and HALOE satellite instruments with the output of SLIMCAT, a chemical transport model. The global HF trends reveal a slowing down in the rate of increase of HF since the 1990s.
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
Sudhanshu Pandey, Sander Houweling, Maarten Krol, Ilse Aben, Frédéric Chevallier, Edward J. Dlugokencky, Luciana V. Gatti, Emanuel Gloor, John B. Miller, Rob Detmers, Toshinobu Machida, and Thomas Röckmann
Atmos. Chem. Phys., 16, 5043–5062, https://doi.org/10.5194/acp-16-5043-2016, https://doi.org/10.5194/acp-16-5043-2016, 2016
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This study investigates the constraint provided by measurements of Xratio (XCH4/XCO2) from space on surface fluxes of CH4 and CO2. We apply the ratio inversion method described in Pandey et al. (2015) to Xratio retrievals from the GOSAT with the TM5-4DVAR inverse modeling system, to constrain the surface fluxes of CH4 and CO2 for 2009 and 2010. The results are compared to proxy CH4 inversions using model-derived-XCO2 mixing ratios from CarbonTracker and MACC.
Antoine Berchet, Philippe Bousquet, Isabelle Pison, Robin Locatelli, Frédéric Chevallier, Jean-Daniel Paris, Ed J. Dlugokencky, Tuomas Laurila, Juha Hatakka, Yrjo Viisanen, Doug E. J. Worthy, Euan Nisbet, Rebecca Fisher, James France, David Lowry, Viktor Ivakhov, and Ove Hermansen
Atmos. Chem. Phys., 16, 4147–4157, https://doi.org/10.5194/acp-16-4147-2016, https://doi.org/10.5194/acp-16-4147-2016, 2016
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We propose insights based on atmospheric observations around the Arctic circle to evaluate estimates of methane emissions to the atmosphere from the East Siberian Arctic Shelf. Based on a comprehensive statistical analysis of the observations and of high-resolution transport simulations, annual methane emissions from ESAS are estimated to range from 0.0 to 4.5 TgCH4 yr−1, with a maximum in summer and very low emissions in winter.
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.
Scot M. Miller, Roisin Commane, Joe R. Melton, Arlyn E. Andrews, Joshua Benmergui, Edward J. Dlugokencky, Greet Janssens-Maenhout, Anna M. Michalak, Colm Sweeney, and Doug E. J. Worthy
Biogeosciences, 13, 1329–1339, https://doi.org/10.5194/bg-13-1329-2016, https://doi.org/10.5194/bg-13-1329-2016, 2016
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We use atmospheric data from the US and Canada to examine seven wetland methane flux estimates. Relative to existing estimates, we find a methane source that is smaller in magnitude with a broader seasonal cycle. Furthermore, we estimate the largest fluxes over the Hudson Bay Lowlands, a spatial distribution that differs from commonly used remote sensing estimates of wetland location.
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. 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.
R. J. Pope, N. H. Savage, M. P. Chipperfield, C. Ordóñez, and L. S. Neal
Atmos. Chem. Phys., 15, 11201–11215, https://doi.org/10.5194/acp-15-11201-2015, https://doi.org/10.5194/acp-15-11201-2015, 2015
A. Berchet, I. Pison, F. Chevallier, J.-D. Paris, P. Bousquet, J.-L. Bonne, M. Y. Arshinov, B. D. Belan, C. Cressot, D. K. Davydov, E. J. Dlugokencky, A. V. Fofonov, A. Galanin, J. Lavrič, T. Machida, R. Parker, M. Sasakawa, R. Spahni, B. D. Stocker, and J. Winderlich
Biogeosciences, 12, 5393–5414, https://doi.org/10.5194/bg-12-5393-2015, https://doi.org/10.5194/bg-12-5393-2015, 2015
L. Molina, G. Broquet, P. Imbach, F. Chevallier, B. Poulter, D. Bonal, B. Burban, M. Ramonet, L. V. Gatti, S. C. Wofsy, J. W. Munger, E. Dlugokencky, and P. Ciais
Atmos. Chem. Phys., 15, 8423–8438, https://doi.org/10.5194/acp-15-8423-2015, https://doi.org/10.5194/acp-15-8423-2015, 2015
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.
R. J. Pope, M. P. Chipperfield, N. H. Savage, C. Ordóñez, L. S. Neal, L. A. Lee, S. S. Dhomse, N. A. D. Richards, and T. D. Keslake
Atmos. Chem. Phys., 15, 5611–5626, https://doi.org/10.5194/acp-15-5611-2015, https://doi.org/10.5194/acp-15-5611-2015, 2015
S. A. Monks, S. R. Arnold, L. K. Emmons, K. S. Law, S. Turquety, B. N. Duncan, J. Flemming, V. Huijnen, S. Tilmes, J. Langner, J. Mao, Y. Long, J. L. Thomas, S. D. Steenrod, J. C. Raut, C. Wilson, M. P. Chipperfield, G. S. Diskin, A. Weinheimer, H. Schlager, and G. Ancellet
Atmos. Chem. Phys., 15, 3575–3603, https://doi.org/10.5194/acp-15-3575-2015, https://doi.org/10.5194/acp-15-3575-2015, 2015
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Multi-model simulations of Arctic CO, O3 and OH are evaluated using observations. Models show highly variable concentrations but the relative importance of emission regions and types is robust across the models, demonstrating the importance of biomass burning as a source. Idealised tracer experiments suggest that some of the model spread is due to variations in simulated transport from Europe in winter and from Asia throughout the year.
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.
M. P. Langowski, C. von Savigny, J. P. Burrows, W. Feng, J. M. C. Plane, D. R. Marsh, D. Janches, M. Sinnhuber, A. C. Aikin, and P. Liebing
Atmos. Chem. Phys., 15, 273–295, https://doi.org/10.5194/acp-15-273-2015, https://doi.org/10.5194/acp-15-273-2015, 2015
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Global concentration fields of Mg and Mg+ in the Earth's upper mesosphere and lower thermosphere (70-150km) are presented. These are retrieved from SCIAMACHY/Envisat satellite grating spectrometer measurements in limb viewing geometry between 2008 and 2012.
These were compared with WACCM-Mg model results and a large fraction of the available measurement results for these species, and an interpretation of the results is done. The variation of these species during NLC presence is discussed.
M. Alexe, P. Bergamaschi, A. Segers, R. Detmers, A. Butz, O. Hasekamp, S. Guerlet, R. Parker, H. Boesch, C. Frankenberg, R. A. Scheepmaker, E. Dlugokencky, C. Sweeney, S. C. Wofsy, and E. A. Kort
Atmos. Chem. Phys., 15, 113–133, https://doi.org/10.5194/acp-15-113-2015, https://doi.org/10.5194/acp-15-113-2015, 2015
G. D. Hayman, F. M. O'Connor, M. Dalvi, D. B. Clark, N. Gedney, C. Huntingford, C. Prigent, M. Buchwitz, O. Schneising, J. P. Burrows, C. Wilson, N. Richards, and M. Chipperfield
Atmos. Chem. Phys., 14, 13257–13280, https://doi.org/10.5194/acp-14-13257-2014, https://doi.org/10.5194/acp-14-13257-2014, 2014
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Globally, wetlands are a major source of methane, which is the second most important greenhouse gas. We find the JULES wetland methane scheme to perform well in general, although there is a tendency for it to overpredict emissions in the tropics and underpredict them in northern latitudes. Our study highlights novel uses of satellite data as a major tool to constrain land-atmosphere methane flux models in a warming world.
S. J. O'Shea, G. Allen, M. W. Gallagher, K. Bower, S. M. Illingworth, J. B. A. Muller, B. T. Jones, C. J. Percival, S. J-B. Bauguitte, M. Cain, N. Warwick, A. Quiquet, U. Skiba, J. Drewer, K. Dinsmore, E. G. Nisbet, D. Lowry, R. E. Fisher, J. L. France, M. Aurela, A. Lohila, G. Hayman, C. George, D. B. Clark, A. J. Manning, A. D. Friend, and J. Pyle
Atmos. Chem. Phys., 14, 13159–13174, https://doi.org/10.5194/acp-14-13159-2014, https://doi.org/10.5194/acp-14-13159-2014, 2014
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This paper presents airborne measurements of greenhouse gases collected in the European Arctic. Regional scale flux estimates for the northern Scandinavian wetlands are derived. These fluxes are found to be in excellent agreement with coincident surface measurements within the aircraft's sampling domain. This has allowed a significant low bias to be identified in two commonly used process-based land surface models.
A. Fraser, P. I. Palmer, L. Feng, H. Bösch, R. Parker, E. J. Dlugokencky, P. B. Krummel, and R. L. Langenfelds
Atmos. Chem. Phys., 14, 12883–12895, https://doi.org/10.5194/acp-14-12883-2014, https://doi.org/10.5194/acp-14-12883-2014, 2014
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Satellite measurements of CO2 and CH4 can be subject to regional systematic errors that can consequently compromise their ability to infer robust flux estimates of these two gases. We develop a method to use retrieved ratios of CH4 and CO2 that are less affected by systematic error. We show that additional in situ data are needed to anchor these observed ratios so they can simultaneously infer fluxes of CO2 and CH4. We argue the ratio data will provide a more faithful description of true fluxes.
J. J. Harrison, M. P. Chipperfield, A. Dudhia, S. Cai, S. Dhomse, C. D. Boone, and P. F. Bernath
Atmos. Chem. Phys., 14, 11915–11933, https://doi.org/10.5194/acp-14-11915-2014, https://doi.org/10.5194/acp-14-11915-2014, 2014
C. Wilson, M. P. Chipperfield, M. Gloor, and F. Chevallier
Geosci. Model Dev., 7, 2485–2500, https://doi.org/10.5194/gmd-7-2485-2014, https://doi.org/10.5194/gmd-7-2485-2014, 2014
S. S. Dhomse, K. M. Emmerson, G. W. Mann, N. Bellouin, K. S. Carslaw, M. P. Chipperfield, R. Hommel, N. L. Abraham, P. Telford, P. Braesicke, M. Dalvi, C. E. Johnson, F. O'Connor, O. Morgenstern, J. A. Pyle, T. Deshler, J. M. Zawodny, and L. W. Thomason
Atmos. Chem. Phys., 14, 11221–11246, https://doi.org/10.5194/acp-14-11221-2014, https://doi.org/10.5194/acp-14-11221-2014, 2014
L. Kritten, A. Butz, M. P. Chipperfield, M. Dorf, S. Dhomse, R. Hossaini, H. Oelhaf, C. Prados-Roman, G. Wetzel, and K. Pfeilsticker
Atmos. Chem. Phys., 14, 9555–9566, https://doi.org/10.5194/acp-14-9555-2014, https://doi.org/10.5194/acp-14-9555-2014, 2014
M. Maione, F. Graziosi, J. Arduini, F. Furlani, U. Giostra, D. R. Blake, P. Bonasoni, X. Fang, S. A. Montzka, S. J. O'Doherty, S. Reimann, A. Stohl, and M. K. Vollmer
Atmos. Chem. Phys., 14, 9755–9770, https://doi.org/10.5194/acp-14-9755-2014, https://doi.org/10.5194/acp-14-9755-2014, 2014
S. O'Doherty, M. Rigby, J. Mühle, D. J. Ivy, B. R. Miller, D. Young, P. G. Simmonds, S. Reimann, M. K. Vollmer, P. B. Krummel, P. J. Fraser, L. P. Steele, B. Dunse, P. K. Salameh, C. M. Harth, T. Arnold, R. F. Weiss, J. Kim, S. Park, S. Li, C. Lunder, O. Hermansen, N. Schmidbauer, L. X. Zhou, B. Yao, R. H. J. Wang, A. J. Manning, and R. G. Prinn
Atmos. Chem. Phys., 14, 9249–9258, https://doi.org/10.5194/acp-14-9249-2014, https://doi.org/10.5194/acp-14-9249-2014, 2014
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
L. Bruhwiler, E. Dlugokencky, K. Masarie, M. Ishizawa, A. Andrews, J. Miller, C. Sweeney, P. Tans, and D. Worthy
Atmos. Chem. Phys., 14, 8269–8293, https://doi.org/10.5194/acp-14-8269-2014, https://doi.org/10.5194/acp-14-8269-2014, 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
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
S. Houweling, M. Krol, P. Bergamaschi, C. Frankenberg, E. J. Dlugokencky, I. Morino, J. Notholt, V. Sherlock, D. Wunch, V. Beck, C. Gerbig, H. Chen, E. A. Kort, T. Röckmann, and I. Aben
Atmos. Chem. Phys., 14, 3991–4012, https://doi.org/10.5194/acp-14-3991-2014, https://doi.org/10.5194/acp-14-3991-2014, 2014
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
A. E. Andrews, J. D. Kofler, M. E. Trudeau, J. C. Williams, D. H. Neff, K. A. Masarie, D. Y. Chao, D. R. Kitzis, P. C. Novelli, C. L. Zhao, E. J. Dlugokencky, P. M. Lang, M. J. Crotwell, M. L. Fischer, M. J. Parker, J. T. Lee, D. D. Baumann, A. R. Desai, C. O. Stanier, S. F. J. De Wekker, D. E. Wolfe, J. W. Munger, and P. P. Tans
Atmos. Meas. Tech., 7, 647–687, https://doi.org/10.5194/amt-7-647-2014, https://doi.org/10.5194/amt-7-647-2014, 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
A. T. Brown, M. P. Chipperfield, N. A. D. Richards, C. Boone, and P. F. Bernath
Atmos. Chem. Phys., 14, 267–282, https://doi.org/10.5194/acp-14-267-2014, https://doi.org/10.5194/acp-14-267-2014, 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
V. V. S. S. Sarma, A. Lenton, R. M. Law, N. Metzl, P. K. Patra, S. Doney, I. D. Lima, E. Dlugokencky, M. Ramonet, and V. Valsala
Biogeosciences, 10, 7035–7052, https://doi.org/10.5194/bg-10-7035-2013, https://doi.org/10.5194/bg-10-7035-2013, 2013
A. L. Ganesan, A. Chatterjee, R. G. Prinn, C. M. Harth, P. K. Salameh, A. J. Manning, B. D. Hall, J. Mühle, L. K. Meredith, R. F. Weiss, S. O'Doherty, and D. Young
Atmos. Chem. Phys., 13, 10633–10644, https://doi.org/10.5194/acp-13-10633-2013, https://doi.org/10.5194/acp-13-10633-2013, 2013
S. S. Dhomse, M. P. Chipperfield, W. Feng, W. T. Ball, Y. C. Unruh, J. D. Haigh, N. A. Krivova, S. K. Solanki, and A. K. Smith
Atmos. Chem. Phys., 13, 10113–10123, https://doi.org/10.5194/acp-13-10113-2013, https://doi.org/10.5194/acp-13-10113-2013, 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
A. T. Brown, M. P. Chipperfield, S. Dhomse, C. Boone, and P. F. Bernath
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-13-23491-2013, https://doi.org/10.5194/acpd-13-23491-2013, 2013
Revised manuscript has not been submitted
S. Basu, S. Guerlet, A. Butz, S. Houweling, O. Hasekamp, I. Aben, P. Krummel, P. Steele, R. Langenfelds, M. Torn, S. Biraud, B. Stephens, A. Andrews, and D. Worthy
Atmos. Chem. Phys., 13, 8695–8717, https://doi.org/10.5194/acp-13-8695-2013, https://doi.org/10.5194/acp-13-8695-2013, 2013
P. D. Hamer, V. Marécal, R. Hossaini, M. Pirre, N. Warwick, M. Chipperfield, A. A. Samah, N. Harris, A. Robinson, B. Quack, A. Engel, K. Krüger, E. Atlas, K. Subramaniam, D. Oram, Emma C. Leedham Elvidge, G. Mills, K. Pfeilsticker, S. Sala, T. Keber, H. Bönisch, L. K. Peng, M. S. M. Nadzir, P. T. Lim, A. Mujahid, A. Anton, H. Schlager, V. Catoire, G. Krysztofiak, S. Fühlbrügge, M. Dorf, and W. T. Sturges
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-13-20611-2013, https://doi.org/10.5194/acpd-13-20611-2013, 2013
Revised manuscript not accepted
S. Kreycy, C. Camy-Peyret, M. P. Chipperfield, M. Dorf, W. Feng, R. Hossaini, L. Kritten, B. Werner, and K. Pfeilsticker
Atmos. Chem. Phys., 13, 6263–6274, https://doi.org/10.5194/acp-13-6263-2013, https://doi.org/10.5194/acp-13-6263-2013, 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
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
N. A. D. Richards, S. R. Arnold, M. P. Chipperfield, G. Miles, A. Rap, R. Siddans, S. A. Monks, and M. J. Hollaway
Atmos. Chem. Phys., 13, 2331–2345, https://doi.org/10.5194/acp-13-2331-2013, https://doi.org/10.5194/acp-13-2331-2013, 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)
Seasonal, regional, and vertical characteristics of high-carbon-monoxide plumes along with their associated ozone anomalies, as seen by IAGOS between 2002 and 2019
The potential of drone observations to improve air quality predictions by 4D-Var
Process analysis of elevated concentrations of organic acids at Whiteface Mountain, New York
Ozone source attribution in polluted European areas during summer 2017 as simulated with MECO(n)
Opinion: Challenges and needs of tropospheric chemical mechanism development
The atmospheric oxidizing capacity in China – Part 2: Sensitivity to emissions of primary pollutants
Role of chemical production and depositional losses on formaldehyde in the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM)
Review of source analyses of ambient volatile organic compounds considering reactive losses: methods of reducing loss effects, impacts of losses, and sources
Interpreting summertime hourly variation of NO2 columns with implications for geostationary satellite applications
An investigation into atmospheric nitrous acid (HONO) processes in South Korea
Performance evaluation of UKESM1 for surface ozone across the pan-tropics
Constraining light dependency in modeled emissions through comparison to observed biogenic volatile organic compound (BVOC) concentrations in a southeastern US forest
A global re-analysis of regionally resolved emissions and atmospheric mole fractions of SF6 for the period 2005–2021
Tropospheric ozone precursors: global and regional distributions, trends, and variability
The contribution of transport emissions to ozone mixing ratios and methane lifetime in 2015 and 2050 in the Shared Socioeconomic Pathways (SSPs)
Ether and ester formation from peroxy radical recombination: a qualitative reaction channel analysis
ACEIC: a comprehensive anthropogenic chlorine emission inventory for China
Impact of methane and other precursor emission reductions on surface ozone in Europe: scenario analysis using the European Monitoring and Evaluation Programme (EMEP) Meteorological Synthesizing Centre – West (MSC-W) model
Verifying national inventory-based combustion emissions of CO2 across the UK and mainland Europe using satellite observations of atmospheric CO and CO2
An improved estimate of inorganic iodine emissions from the ocean using a coupled surface microlayer box model
Impact of improved representation of volatile organic compound emissions and production of NOx reservoirs on modeled urban ozone production
The effect of different climate and air quality policies in China on in situ ozone production in Beijing
Assessing the relative impacts of satellite ozone and its precursor observations to improve global tropospheric ozone analysis using multiple chemical reanalysis systems
Evaluating present-day and future impacts of agricultural ammonia emissions on atmospheric chemistry and climate
Enhancing long-term trend simulation of the global tropospheric hydroxyl (TOH) and its drivers from 2005 to 2019: a synergistic integration of model simulations and satellite observations
Intercomparison of GEOS-Chem and CAM-chem tropospheric oxidant chemistry within the Community Earth System Model version 2 (CESM2)
Development of a detailed gaseous oxidation scheme of naphthalene for secondary organic aerosol (SOA) formation and speciation
Air pollution satellite-based CO2 emission inversion: system evaluation, sensitivity analysis, and future perspective
Anthropogenic emission controls reduce summertime ozone-temperature sensitivity in the United States
Large contributions of soil emissions to the atmospheric nitrogen budget and their impacts on air quality and temperature rise in North China
Why did ozone concentrations remain high during Shanghai's static management? A statistical and radical-chemistry perspective
Impact of introducing electric vehicles on ground-level O3 and PM2.5 in the Greater Tokyo Area: Yearly trends and the importance of changes in the Urban Heat Island effect
Revising VOC emissions speciation improves the simulation of global background ethane and propane
Changes in South American surface ozone trends: exploring the influences of precursors and extreme events
Evaluating NOx stack plume emissions using a high-resolution atmospheric chemistry model and satellite-derived NO2 columns
NOx emissions in France in 2019–2021 as estimated by the high-spatial-resolution assimilation of TROPOMI NO2 observations
Urban ozone formation and sensitivities to volatile chemical products, cooking emissions, and NOx across the Los Angeles Basin
Aggravated surface O3 pollution primarily driven by meteorological variations in China during the 2020 COVID-19 pandemic lockdown period
Identifying decadal trends in deweathered concentrations of criteria air pollutants in Canadian urban atmospheres with machine learning approaches
Evaluation of modelled versus observed non-methane volatile organic compounds at European Monitoring and Evaluation Programme sites in Europe
Constraining non-methane VOC emissions with TROPOMI HCHO observations: impact on summertime ozone simulation in August 2022 in China
Insights on ozone pollution control in urban areas by decoupling meteorological factors based on machine learning
Revealing the significant acceleration of hydrofluorocarbon (HFC) emissions in eastern Asia through long-term atmospheric observations
Interpreting Geostationary Environment Monitoring Spectrometer (GEMS) geostationary satellite observations of the diurnal variation in nitrogen dioxide (NO2) over East Asia
An intercomparison of satellite, airborne, and ground-level observations with WRF–CAMx simulations of NO2 columns over Houston, Texas, during the September 2021 TRACER-AQ campaign
Investigating processes influencing simulation of local Arctic wintertime anthropogenic pollution in Fairbanks, Alaska during ALPACA-2022
Interannual variability of summertime formaldehyde (HCHO) vertical column density and its main drivers at northern high latitudes
The impact of multi-decadal changes in VOC speciation on urban ozone chemistry: a case study in Birmingham, United Kingdom
Technical note: Challenges in detecting free tropospheric ozone trends in a sparsely sampled environment
Combined assimilation of NOAA surface and MIPAS satellite observations to constrain the global budget of carbonyl sulfide
Thibaut Lebourgeois, Bastien Sauvage, Pawel Wolff, Béatrice Josse, Virginie Marécal, Yasmine Bennouna, Romain Blot, Damien Boulanger, Hannah Clark, Jean-Marc Cousin, Philippe Nedelec, and Valérie Thouret
Atmos. Chem. Phys., 24, 13975–14004, https://doi.org/10.5194/acp-24-13975-2024, https://doi.org/10.5194/acp-24-13975-2024, 2024
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Our study examines intense-carbon-monoxide (CO) pollution events measured by commercial aircraft from the In-service Aircraft for a Global Observing System (IAGOS) research infrastructure. We combine these measurements with the SOFT-IO model to trace the origin of the observed CO. A comprehensive analysis of the geographical origin, source type, seasonal variation, and ozone levels of these pollution events is provided.
Hassnae Erraji, Philipp Franke, Astrid Lampert, Tobias Schuldt, Ralf Tillmann, Andreas Wahner, and Anne Caroline Lange
Atmos. Chem. Phys., 24, 13913–13934, https://doi.org/10.5194/acp-24-13913-2024, https://doi.org/10.5194/acp-24-13913-2024, 2024
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Four-dimensional variational data assimilation allows for the simultaneous optimisation of initial values and emission rates by using trace-gas profiles from drone observations in a regional air quality model. Assimilated profiles positively impact the representation of air pollutants in the model by improving their vertical distribution and ground-level concentrations. This case study highlights the potential of drone data to enhance air quality analyses including local emission evaluation.
Christopher Lawrence, Mary Barth, John Orlando, Paul Casson, Richard Brandt, Daniel Kelting, Elizabeth Yerger, and Sara Lance
Atmos. Chem. Phys., 24, 13693–13713, https://doi.org/10.5194/acp-24-13693-2024, https://doi.org/10.5194/acp-24-13693-2024, 2024
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This work uses chemical transport and box modeling to study the gas- and aqueous-phase production of organic acid concentrations measured in cloud water at the summit of Whiteface Mountain on 1 July 2018. Isoprene was the major source of formic, acetic, and oxalic acid. Gas-phase chemistry greatly underestimated formic and acetic acid, indicating missing sources, while cloud chemistry was a key source of oxalic acid. More studies of organic acids are required to better constrain their sources.
Markus Kilian, Volker Grewe, Patrick Jöckel, Astrid Kerkweg, Mariano Mertens, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 24, 13503–13523, https://doi.org/10.5194/acp-24-13503-2024, https://doi.org/10.5194/acp-24-13503-2024, 2024
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Anthropogenic emissions are a major source of precursors of tropospheric ozone. As ozone formation is highly non-linear, we apply a global–regional chemistry–climate model with a source attribution method (tagging) to quantify the contribution of anthropogenic emissions to ozone. Our analysis shows that the contribution of European anthropogenic emissions largely increases during large ozone periods, indicating that emissions from these sectors drive ozone values.
Barbara Ervens, Andrew Rickard, Bernard Aumont, William P. L. Carter, Max McGillen, Abdelwahid Mellouki, John Orlando, Bénédicte Picquet-Varrault, Paul Seakins, William R. Stockwell, Luc Vereecken, and Timothy J. Wallington
Atmos. Chem. Phys., 24, 13317–13339, https://doi.org/10.5194/acp-24-13317-2024, https://doi.org/10.5194/acp-24-13317-2024, 2024
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Chemical mechanisms describe the chemical processes in atmospheric models that are used to describe the changes in the atmospheric composition. Therefore, accurate chemical mechanisms are necessary to predict the evolution of air pollution and climate change. The article describes all steps that are needed to build chemical mechanisms and discusses the advances and needs of experimental and theoretical research activities needed to build reliable chemical mechanisms.
Jianing Dai, Guy P. Brasseur, Mihalis Vrekoussis, Maria Kanakidou, Kun Qu, Yijuan Zhang, Hongliang Zhang, and Tao Wang
Atmos. Chem. Phys., 24, 12943–12962, https://doi.org/10.5194/acp-24-12943-2024, https://doi.org/10.5194/acp-24-12943-2024, 2024
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This paper employs a regional chemical transport model to quantify the sensitivity of air pollutants and photochemical parameters to specified emission reductions in China for representative winter and summer conditions. The study provides insights into further air quality control in China with reduced primary emissions.
T. Nash Skipper, Emma L. D'Ambro, Forwood C. Wiser, V. Faye McNeill, Rebecca H. Schwantes, Barron H. Henderson, Ivan R. Piletic, Colleen B. Baublitz, Jesse O. Bash, Andrew R. Whitehill, Lukas C. Valin, Asher P. Mouat, Jennifer Kaiser, Glenn M. Wolfe, Jason M. St. Clair, Thomas F. Hanisco, Alan Fried, Bryan K. Place, and Havala O.T. Pye
Atmos. Chem. Phys., 24, 12903–12924, https://doi.org/10.5194/acp-24-12903-2024, https://doi.org/10.5194/acp-24-12903-2024, 2024
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We develop the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM) version 2 to improve predictions of formaldehyde in ambient air compared to satellite-, aircraft-, and ground-based observations. With the updated chemistry, we estimate the cancer risk from inhalation exposure to ambient formaldehyde across the contiguous USA and predict that 40 % of this risk is controllable through reductions in anthropogenic emissions of nitrogen oxides and reactive organic carbon.
Baoshuang Liu, Yao Gu, Yutong Wu, Qili Dai, Shaojie Song, Yinchang Feng, and Philip K. Hopke
Atmos. Chem. Phys., 24, 12861–12879, https://doi.org/10.5194/acp-24-12861-2024, https://doi.org/10.5194/acp-24-12861-2024, 2024
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Reactive loss of volatile organic compounds (VOCs) is a long-term issue yet to be resolved in VOC source analyses. We assess common methods of, and existing issues in, reducing losses, impacts of losses, and sources in current source analyses. We offer a potential supporting role for solving issues of VOC conversion. Source analyses of consumed VOCs that reacted to produce ozone and secondary organic aerosols can play an important role in the effective control of secondary pollution in air.
Deepangsu Chatterjee, Randall V. Martin, Chi Li, Dandan Zhang, Haihui Zhu, Daven K. Henze, James H. Crawford, Ronald C. Cohen, Lok N. Lamsal, and Alexander M. Cede
Atmos. Chem. Phys., 24, 12687–12706, https://doi.org/10.5194/acp-24-12687-2024, https://doi.org/10.5194/acp-24-12687-2024, 2024
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We investigate the hourly variation of NO2 columns and surface concentrations by applying the GEOS-Chem model to interpret aircraft and ground-based measurements over the US and Pandora sun photometer measurements over the US, Europe, and Asia. Corrections to the Pandora columns and finer model resolution improve the modeled representation of the summertime hourly variation of total NO2 columns to explain the weaker hourly variation in NO2 columns than at the surface.
Kiyeon Kim, Kyung Man Han, Chul Han Song, Hyojun Lee, Ross Beardsley, Jinhyeok Yu, Greg Yarwood, Bonyoung Koo, Jasper Madalipay, Jung-Hun Woo, and Seogju Cho
Atmos. Chem. Phys., 24, 12575–12593, https://doi.org/10.5194/acp-24-12575-2024, https://doi.org/10.5194/acp-24-12575-2024, 2024
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We incorporated each HONO process into the current CMAQ modeling framework to enhance the accuracy of HONO mixing ratio predictions. These results expand our understanding of HONO photochemistry and identify crucial sources of HONO that impact the total HONO budget in Seoul, South Korea. Through this investigation, we contribute to resolving discrepancies in understanding chemical transport models, with implications for better air quality management and environmental protection in the region.
Flossie Brown, Gerd Folberth, Stephen Sitch, Paulo Artaxo, Marijn Bauters, Pascal Boeckx, Alexander W. Cheesman, Matteo Detto, Ninong Komala, Luciana Rizzo, Nestor Rojas, Ines dos Santos Vieira, Steven Turnock, Hans Verbeeck, and Alfonso Zambrano
Atmos. Chem. Phys., 24, 12537–12555, https://doi.org/10.5194/acp-24-12537-2024, https://doi.org/10.5194/acp-24-12537-2024, 2024
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Ozone is a pollutant that is detrimental to human and plant health. Ozone monitoring sites in the tropics are limited, so models are often used to understand ozone exposure. We use measurements from the tropics to evaluate ozone from the UK Earth system model, UKESM1. UKESM1 is able to capture the pattern of ozone in the tropics, except in southeast Asia, although it systematically overestimates it at all sites. This work highlights that UKESM1 can capture seasonal and hourly variability.
Namrata Shanmukh Panji, Deborah F. McGlynn, Laura E. R. Barry, Todd M. Scanlon, Manuel T. Lerdau, Sally E. Pusede, and Gabriel Isaacman-VanWertz
Atmos. Chem. Phys., 24, 12495–12507, https://doi.org/10.5194/acp-24-12495-2024, https://doi.org/10.5194/acp-24-12495-2024, 2024
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Climate change will bring about changes in parameters that are currently used in global-scale models to calculate biogenic emissions. This study seeks to understand the factors driving these models by comparing long-term datasets of biogenic compounds to modeled emissions. We note that the light-dependent fractions currently used in models do not accurately represent regional observations. We provide evidence for the time-dependent variation in this parameter for future modifications to models.
Martin Vojta, Andreas Plach, Saurabh Annadate, Sunyoung Park, Gawon Lee, Pallav Purohit, Florian Lindl, Xin Lan, Jens Mühle, Rona L. Thompson, and Andreas Stohl
Atmos. Chem. Phys., 24, 12465–12493, https://doi.org/10.5194/acp-24-12465-2024, https://doi.org/10.5194/acp-24-12465-2024, 2024
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We constrain the global emissions of the very potent greenhouse gas sulfur hexafluoride (SF6) between 2005 and 2021. We show that SF6 emissions are decreasing in the USA and in the EU, while they are substantially growing in China, leading overall to an increasing global emission trend. The national reports for the USA, EU, and China all underestimated their SF6 emissions. However, stringent mitigation measures can successfully reduce SF6 emissions, as can be seen in the EU emission trend.
Yasin Elshorbany, Jerald R. Ziemke, Sarah Strode, Hervé Petetin, Kazuyuki Miyazaki, Isabelle De Smedt, Kenneth Pickering, Rodrigo J. Seguel, Helen Worden, Tamara Emmerichs, Domenico Taraborrelli, Maria Cazorla, Suvarna Fadnavis, Rebecca R. Buchholz, Benjamin Gaubert, Néstor Y. Rojas, Thiago Nogueira, Thérèse Salameh, and Min Huang
Atmos. Chem. Phys., 24, 12225–12257, https://doi.org/10.5194/acp-24-12225-2024, https://doi.org/10.5194/acp-24-12225-2024, 2024
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We investigated tropospheric ozone spatial variability and trends from 2005 to 2019 and related those to ozone precursors on global and regional scales. We also investigate the spatiotemporal characteristics of the ozone formation regime in relation to ozone chemical sources and sinks. Our analysis is based on remote sensing products of the tropospheric column of ozone and its precursors, nitrogen dioxide, formaldehyde, and total column CO, as well as ozonesonde data and model simulations.
Mariano Mertens, Sabine Brinkop, Phoebe Graf, Volker Grewe, Johannes Hendricks, Patrick Jöckel, Anna Lanteri, Sigrun Matthes, Vanessa S. Rieger, Mattia Righi, and Robin N. Thor
Atmos. Chem. Phys., 24, 12079–12106, https://doi.org/10.5194/acp-24-12079-2024, https://doi.org/10.5194/acp-24-12079-2024, 2024
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We quantified the contributions of land transport, shipping, and aviation emissions to tropospheric ozone; its radiative forcing; and the reductions of the methane lifetime using chemistry-climate model simulations. The contributions were analysed for the conditions of 2015 and for three projections for the year 2050. The results highlight the challenges of mitigating ozone formed by emissions of the transport sector, caused by the non-linearitiy of the ozone chemistry and the long lifetime.
Lauri Franzon, Marie Camredon, Richard Valorso, Bernard Aumont, and Theo Kurtén
Atmos. Chem. Phys., 24, 11679–11699, https://doi.org/10.5194/acp-24-11679-2024, https://doi.org/10.5194/acp-24-11679-2024, 2024
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In this article we investigate the formation of large, sticky molecules from various organic compounds entering the atmosphere as primary emissions and the degree to which these processes may contribute to organic aerosol particle mass. More specifically, we qualitatively investigate a recently discovered chemical reaction channel for one of the most important short-lived radical compounds, peroxy radicals, and discover which of these reactions are most atmospherically important.
Siting Li, Yiming Liu, Yuqi Zhu, Yinbao Jin, Yingying Hong, Ao Shen, Yifei Xu, Haofan Wang, Haichao Wang, Xiao Lu, Shaojia Fan, and Qi Fan
Atmos. Chem. Phys., 24, 11521–11544, https://doi.org/10.5194/acp-24-11521-2024, https://doi.org/10.5194/acp-24-11521-2024, 2024
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This study establishes an inventory of anthropogenic chlorine emissions in China in 2019 with expanded species (HCl, Cl-, Cl2, HOCl) and sources (41 specific sources). The inventory is validated by a modeling study against the observations. This study enhances the understanding of anthropogenic chlorine emissions in the atmosphere, identifies key sources, and provides scientific support for pollution control and climate change.
Willem E. van Caspel, Zbigniew Klimont, Chris Heyes, and Hilde Fagerli
Atmos. Chem. Phys., 24, 11545–11563, https://doi.org/10.5194/acp-24-11545-2024, https://doi.org/10.5194/acp-24-11545-2024, 2024
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Methane in the atmosphere contributes to the production of ozone gas – an air pollutant and greenhouse gas. Our results highlight that simultaneous reductions in methane emissions help avoid offsetting the air pollution benefits already achieved by the already-approved precursor emission reductions by 2050 in the European Monitoring and Evaluation Programme region, while also playing an important role in bringing air pollution further down towards World Health Organization guideline limits.
Tia R. Scarpelli, Paul I. Palmer, Mark Lunt, Ingrid Super, and Arjan Droste
Atmos. Chem. Phys., 24, 10773–10791, https://doi.org/10.5194/acp-24-10773-2024, https://doi.org/10.5194/acp-24-10773-2024, 2024
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Under the Paris Agreement, countries must track their anthropogenic greenhouse gas emissions. This study describes a method to determine self-consistent estimates for combustion emissions and natural fluxes of CO2 from atmospheric data. We report consistent estimates inferred using this approach from satellite data and ground-based data over Europe, suggesting that satellite data can be used to determine national anthropogenic CO2 emissions for countries where ground-based CO2 data are absent.
Ryan J. Pound, Lucy V. Brown, Mat J. Evans, and Lucy J. Carpenter
Atmos. Chem. Phys., 24, 9899–9921, https://doi.org/10.5194/acp-24-9899-2024, https://doi.org/10.5194/acp-24-9899-2024, 2024
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Iodine-mediated loss of ozone to the ocean surface and the subsequent emission of iodine species has a large effect on the troposphere. Here we combine recent experimental insights to develop a box model of the process, which we then parameterize and incorporate into the GEOS-Chem transport model. We find that these new insights have a small impact on the total emission of iodine but significantly change its distribution.
Katherine R. Travis, Benjamin A. Nault, James H. Crawford, Kelvin H. Bates, Donald R. Blake, Ronald C. Cohen, Alan Fried, Samuel R. Hall, L. Gregory Huey, Young Ro Lee, Simone Meinardi, Kyung-Eun Min, Isobel J. Simpson, and Kirk Ullman
Atmos. Chem. Phys., 24, 9555–9572, https://doi.org/10.5194/acp-24-9555-2024, https://doi.org/10.5194/acp-24-9555-2024, 2024
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Human activities result in the emission of volatile organic compounds (VOCs) that contribute to air pollution. Detailed VOC measurements were taken during a field study in South Korea. When compared to VOC inventories, large discrepancies showed underestimates from chemical products, liquefied petroleum gas, and long-range transport. Improved emissions and chemistry of these VOCs better described urban pollution. The new chemical scheme is relevant to urban areas and other VOC sources.
Beth S. Nelson, Zhenze Liu, Freya A. Squires, Marvin Shaw, James R. Hopkins, Jacqueline F. Hamilton, Andrew R. Rickard, Alastair C. Lewis, Zongbo Shi, and James D. Lee
Atmos. Chem. Phys., 24, 9031–9044, https://doi.org/10.5194/acp-24-9031-2024, https://doi.org/10.5194/acp-24-9031-2024, 2024
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The impact of combined air quality and carbon neutrality policies on O3 formation in Beijing was investigated. Emissions inventory data were used to estimate future pollutant mixing ratios relative to ground-level observations. O3 production was found to be most sensitive to changes in alkenes, but large reductions in less reactive compounds led to larger reductions in future O3 production. This study highlights the importance of understanding the emissions of organic pollutants.
Takashi Sekiya, Emanuele Emili, Kazuyuki Miyazaki, Antje Inness, Zhen Qu, R. Bradley Pierce, Dylan Jones, Helen Worden, William Y. Y. Cheng, Vincent Huijnen, and Gerbrand Koren
EGUsphere, https://doi.org/10.5194/egusphere-2024-2426, https://doi.org/10.5194/egusphere-2024-2426, 2024
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Five global chemical reanalysis datasets were used to assess the relative impacts of assimilating satellite ozone and its precursors measurements on tropospheric ozone analyses for 2010. The multiple reanalysis system comparison allows for evaluating dependency of the impacts on different reanalysis systems. The results suggested the importance of satellite ozone and its precursor measurements for improving ozone analysis in the whole troposphere, with varying the magnitudes among the systems.
Maureen Beaudor, Didier Hauglustaine, Juliette Lathière, Martin Van Damme, Lieven Clarisse, and Nicolas Vuichard
EGUsphere, https://doi.org/10.5194/egusphere-2024-2022, https://doi.org/10.5194/egusphere-2024-2022, 2024
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Agriculture is the biggest ammonia (NH3) source, impacting air quality, climate, and ecosystems. Because of food demand, NH3 emissions are projected to rise by 2100. Using a global model, we analyzed the impact of present and future NH3 emissions generated from a land model. Our results show improved ammonia patterns compared to a reference inventory. Future scenarios predict up to 70 % increase in global NH3 burden, significant changes in radiative forcing, and could significantly elevate N2O.
Amir H. Souri, Bryan N. Duncan, Sarah A. Strode, Daniel C. Anderson, Michael E. Manyin, Junhua Liu, Luke D. Oman, Zhen Zhang, and Brad Weir
Atmos. Chem. Phys., 24, 8677–8701, https://doi.org/10.5194/acp-24-8677-2024, https://doi.org/10.5194/acp-24-8677-2024, 2024
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We explore a new method of using the wealth of information obtained from satellite observations of Aura OMI NO2, HCHO, and MERRA-2 reanalysis in NASA’s GEOS model equipped with an efficient tropospheric OH (TOH) estimator to enhance the representation of TOH spatial distribution and its long-term trends. This new framework helps us pinpoint regional inaccuracies in TOH and differentiate between established prior knowledge and newly acquired information from satellites on TOH trends.
Haipeng Lin, Louisa K. Emmons, Elizabeth W. Lundgren, Laura Hyesung Yang, Xu Feng, Ruijun Dang, Shixian Zhai, Yunxiao Tang, Makoto M. Kelp, Nadia K. Colombi, Sebastian D. Eastham, Thibaud M. Fritz, and Daniel J. Jacob
Atmos. Chem. Phys., 24, 8607–8624, https://doi.org/10.5194/acp-24-8607-2024, https://doi.org/10.5194/acp-24-8607-2024, 2024
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Tropospheric ozone is a major air pollutant, a greenhouse gas, and a major indicator of model skill. Global atmospheric chemistry models show large differences in simulations of tropospheric ozone, but isolating sources of differences is complicated by different model environments. By implementing the GEOS-Chem model side by side to CAM-chem within a common Earth system model, we identify and evaluate specific differences between the two models and their impacts on key chemical species.
Victor Lannuque and Karine Sartelet
Atmos. Chem. Phys., 24, 8589–8606, https://doi.org/10.5194/acp-24-8589-2024, https://doi.org/10.5194/acp-24-8589-2024, 2024
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Large uncertainties remain in understanding secondary organic aerosol (SOA) formation and speciation from naphthalene oxidation. This study details the development of the first near-explicit chemical scheme for naphthalene oxidation by OH, which includes kinetic and mechanistic data, and is able to reproduce most of the experimentally identified products in both gas and particle phases.
Hui Li, Jiaxin Qiu, and Bo Zheng
EGUsphere, https://doi.org/10.5194/egusphere-2024-1986, https://doi.org/10.5194/egusphere-2024-1986, 2024
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We conduct a sensitivity analysis on various factors including prior, model resolution, satellite constraint, and inversion system configuration to assess the vulnerability of emission estimates across temporal, sectoral, and regional dimensions. Our analysis first reveals the robustness of emissions estimated by this air pollution satellite sensor-based CO2 emission inversion system, with relative change between tests and Base inversion below 4.0 % for national annual NOx and CO2 emissions.
Shuai Li, Xiao Lu, and Haolin Wang
EGUsphere, https://doi.org/10.5194/egusphere-2024-1889, https://doi.org/10.5194/egusphere-2024-1889, 2024
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We report that the summertime ozone-temperature sensitivity decreased by 50 % from 3.0 ppbv/K in 1990 to 1.5 ppb/K in 2021 in the US. GEOS-Chem simulations show that anthropogenic NOx emission reduction is the dominant driver of the ozone-temperature sensitivity decline, through influencing both the temperature-direct and temperature-indirect processes. Reduced ozone-temperature sensitivity has decreased the ozone enhancement from low to high temperatures by an average of 6.8 ppbv across the US.
Tong Sha, Siyu Yang, Qingcai Chen, Liangqing Li, Xiaoyan Ma, Yan-Lin Zhang, Zhaozhong Feng, K. Folkert Boersma, and Jun Wang
Atmos. Chem. Phys., 24, 8441–8455, https://doi.org/10.5194/acp-24-8441-2024, https://doi.org/10.5194/acp-24-8441-2024, 2024
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Using an updated soil reactive nitrogen emission scheme in the Unified Inputs for Weather Research and Forecasting coupled with Chemistry (UI-WRF-Chem) model, we investigate the role of soil NO and HONO (Nr) emissions in air quality and temperature in North China. Contributions of soil Nr emissions to O3 and secondary pollutants are revealed, exceeding effects of soil NOx or HONO emission. Soil Nr emissions play an important role in mitigating O3 pollution and addressing climate change.
Jian Zhu, Shanshan Wang, Chuanqi Gu, Zhiwen Jiang, Sanbao Zhang, Ruibin Xue, Yuhao Yan, and Bin Zhou
Atmos. Chem. Phys., 24, 8383–8395, https://doi.org/10.5194/acp-24-8383-2024, https://doi.org/10.5194/acp-24-8383-2024, 2024
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In 2022, Shanghai implemented city-wide static management measures during the high-ozone season in April and May, providing a chance to study ozone pollution control. Despite significant emissions reductions, ozone levels increased by 23 %. Statistically, the number of days with higher ozone diurnal variation types increased during the lockdown period. The uneven decline in VOC and NO2 emissions led to heightened photochemical processes, resulting in the observed ozone level rise.
Hiroo Hata, Norifumi Mizushima, and Tomohiko Ihara
EGUsphere, https://doi.org/10.5194/egusphere-2024-1961, https://doi.org/10.5194/egusphere-2024-1961, 2024
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The introduction of battery electric vehicles (BEV) is expected to reduce the primary air pollutants from vehicular exhaust and evaporative emissions while reducing the anthropogenic heat produced by vehicles, ultimately decreasing the urban heat island effect (UHI). This study revealed the impact of introducing BEVs on the decrease in UHI and the effects of BEVs on the formation of tropospheric ozone and fine particulate matter in the Greater Tokyo Area of Japan.
Matthew J. Rowlinson, Mat J. Evans, Lucy J. Carpenter, Katie A. Read, Shalini Punjabi, Adedayo Adedeji, Luke Fakes, Ally Lewis, Ben Richmond, Neil Passant, Tim Murrells, Barron Henderson, Kelvin H. Bates, and Detlev Helmig
Atmos. Chem. Phys., 24, 8317–8342, https://doi.org/10.5194/acp-24-8317-2024, https://doi.org/10.5194/acp-24-8317-2024, 2024
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Ethane and propane are volatile organic compounds emitted from human activities which help to form ozone, a pollutant and greenhouse gas, and also affect the chemistry of the lower atmosphere. Atmospheric models tend to do a poor job of reproducing the abundance of these compounds in the atmosphere. By using regional estimates of their emissions, rather than globally consistent estimates, we can significantly improve the simulation of ethane in the model and make some improvement for propane.
Rodrigo J. Seguel, Lucas Castillo, Charlie Opazo, Néstor Y. Rojas, Thiago Nogueira, María Cazorla, Mario Gavidia-Calderón, Laura Gallardo, René Garreaud, Tomás Carrasco-Escaff, and Yasin Elshorbany
Atmos. Chem. Phys., 24, 8225–8242, https://doi.org/10.5194/acp-24-8225-2024, https://doi.org/10.5194/acp-24-8225-2024, 2024
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Trends of surface ozone were examined across South America. Our findings indicate that ozone trends in major South American cities either increase or remain steady, with no signs of decline. The upward trends can be attributed to chemical regimes that efficiently convert nitric oxide into nitrogen dioxide. Additionally, our results suggest a climate penalty for ozone driven by meteorological conditions that favor wildfire propagation in Chile and extensive heat waves in southern Brazil.
Maarten Krol, Bart van Stratum, Isidora Anglou, and Klaas Folkert Boersma
Atmos. Chem. Phys., 24, 8243–8262, https://doi.org/10.5194/acp-24-8243-2024, https://doi.org/10.5194/acp-24-8243-2024, 2024
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This paper presents detailed plume simulations of nitrogen oxides and carbon dioxide that are emitted from four large industrial facilities world-wide. Results from the high-resolution simulations that include atmospheric chemistry are compared to nitrogen dioxide observations from satellites. We find good performance of the model and show that common assumptions that are used in simplified models need revision. This work is important for the monitoring of emissions using satellite data.
Robin Plauchu, Audrey Fortems-Cheiney, Grégoire Broquet, Isabelle Pison, Antoine Berchet, Elise Potier, Gaëlle Dufour, Adriana Coman, Dilek Savas, Guillaume Siour, and Henk Eskes
Atmos. Chem. Phys., 24, 8139–8163, https://doi.org/10.5194/acp-24-8139-2024, https://doi.org/10.5194/acp-24-8139-2024, 2024
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This study uses the Community Inversion Framework and CHIMERE model to assess the potential of TROPOMI-S5P PAL NO2 tropospheric column data to estimate NOx emissions in France (2019–2021). Results show a 3 % decrease in average emissions compared to the 2016 CAMS-REG/INS, lower than the 14 % decrease from CITEPA. The study highlights challenges in capturing emission anomalies due to limited data coverage and error levels but shows promise for local inventory improvements.
Chelsea E. Stockwell, Matthew M. Coggon, Rebecca H. Schwantes, Colin Harkins, Bert Verreyken, Congmeng Lyu, Qindan Zhu, Lu Xu, Jessica B. Gilman, Aaron Lamplugh, Jeff Peischl, Michael A. Robinson, Patrick R. Veres, Meng Li, Andrew W. Rollins, Kristen Zuraski, Sunil Baidar, Shang Liu, Toshihiro Kuwayama, Steven S. Brown, Brian C. McDonald, and Carsten Warneke
EGUsphere, https://doi.org/10.5194/egusphere-2024-1899, https://doi.org/10.5194/egusphere-2024-1899, 2024
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In urban areas, emissions from everyday products like paints, cleaners, and personal care products, along with non-traditional sources such as cooking are important sources that impact air quality. This study used a model to evaluate how these emissions impact ozone in the Los Angeles Basin, and quantifies the impact of gaseous cooking emissions for the first time. Accurate representation of these and other man-made sources in inventories is crucial to inform effective air quality policies.
Zhendong Lu, Jun Wang, Yi Wang, Daven K. Henze, Xi Chen, Tong Sha, and Kang Sun
Atmos. Chem. Phys., 24, 7793–7813, https://doi.org/10.5194/acp-24-7793-2024, https://doi.org/10.5194/acp-24-7793-2024, 2024
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In contrast with past work showing that the reduction of emissions was the dominant factor for the nationwide increase of surface O3 during the lockdown in China, this study finds that the variation in meteorology (temperature and other parameters) plays a more important role. This result is obtained through sensitivity simulations using a chemical transport model constrained by satellite (TROPOMI) data and calibrated with surface observations.
Xiaohong Yao and Leiming Zhang
Atmos. Chem. Phys., 24, 7773–7791, https://doi.org/10.5194/acp-24-7773-2024, https://doi.org/10.5194/acp-24-7773-2024, 2024
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This study investigates long-term trends of criteria air pollutants, including NO2, CO, SO2, O3 and PM2.5, and NO2+O3 measured in 10 Canadian cities during the last 2 to 3 decades. We also investigate associated driving forces in terms of emission reductions, perturbations from varying weather conditions and large-scale wildfires, as well as changes in O3 sources and sinks.
Yao Ge, Sverre Solberg, Mathew R. Heal, Stefan Reimann, Willem van Caspel, Bryan Hellack, Thérèse Salameh, and David Simpson
Atmos. Chem. Phys., 24, 7699–7729, https://doi.org/10.5194/acp-24-7699-2024, https://doi.org/10.5194/acp-24-7699-2024, 2024
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Atmospheric volatile organic compounds (VOCs) constitute many species, acting as precursors to ozone and aerosol. Given the uncertainties in VOC emissions, lack of evaluation studies, and recent changes in emissions, this work adapts the EMEP MSC-W to evaluate emission inventories in Europe. We focus on the varying agreement between modelled and measured VOCs across different species and underscore potential inaccuracies in total and sector-specific emission estimates.
Shuzhuang Feng, Fei Jiang, Tianlu Qian, Nan Wang, Mengwei Jia, Songci Zheng, Jiansong Chen, Fang Ying, and Weimin Ju
Atmos. Chem. Phys., 24, 7481–7498, https://doi.org/10.5194/acp-24-7481-2024, https://doi.org/10.5194/acp-24-7481-2024, 2024
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We developed a multi-air-pollutant inversion system to estimate non-methane volatile organic compound (NMVOC) emissions using TROPOMI formaldehyde retrievals. We found that the inversion significantly improved formaldehyde simulations and reduced NMVOC emission uncertainties. The optimized NMVOC emissions effectively corrected the overestimation of O3 levels, mainly by decreasing the rate of the RO2 + NO reaction and increasing the rate of the NO2 + OH reaction.
Yuqing Qiu, Xin Li, Wenxuan Chai, Yi Liu, Mengdi Song, Xudong Tian, Qiaoli Zou, Wenjun Lou, Wangyao Zhang, Juan Li, and Yuanhang Zhang
EGUsphere, https://doi.org/10.5194/egusphere-2024-1576, https://doi.org/10.5194/egusphere-2024-1576, 2024
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The chemical reactions of ozone (O3) formation are related to meteorology and local emissions. Here, a random forest approach was used to eliminate the effects of meteorological factors (dispersion or transport) on O3 and its precursors. Variations in the sensitivity of O3 formation and the apportionment of emission sources were revealed after meteorological normalization. Our results suggest that meteorological variations should be considered when diagnosing O3 formation.
Haklim Choi, Alison L. Redington, Hyeri Park, Jooil Kim, Rona L. Thompson, Jens Mühle, Peter K. Salameh, Christina M. Harth, Ray F. Weiss, Alistair J. Manning, and Sunyoung Park
Atmos. Chem. Phys., 24, 7309–7330, https://doi.org/10.5194/acp-24-7309-2024, https://doi.org/10.5194/acp-24-7309-2024, 2024
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We analyzed with an inversion model the atmospheric abundance of hydrofluorocarbons (HFCs), potent greenhouse gases, from 2008 to 2020 at Gosan station in South Korea and revealed a significant increase in emissions, especially from eastern China and Japan. This increase contradicts reported data, underscoring the need for accurate monitoring and reporting. Our findings are crucial for understanding and managing global HFCs emissions, highlighting the importance of efforts to reduce HFCs.
Laura Hyesung Yang, Daniel J. Jacob, Ruijun Dang, Yujin J. Oak, Haipeng Lin, Jhoon Kim, Shixian Zhai, Nadia K. Colombi, Drew C. Pendergrass, Ellie Beaudry, Viral Shah, Xu Feng, Robert M. Yantosca, Heesung Chong, Junsung Park, Hanlim Lee, Won-Jin Lee, Soontae Kim, Eunhye Kim, Katherine R. Travis, James H. Crawford, and Hong Liao
Atmos. Chem. Phys., 24, 7027–7039, https://doi.org/10.5194/acp-24-7027-2024, https://doi.org/10.5194/acp-24-7027-2024, 2024
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The Geostationary Environment Monitoring Spectrometer (GEMS) provides hourly measurements of NO2. We use the chemical transport model to find how emissions, chemistry, and transport drive the changes in NO2 observed by GEMS at different times of the day. In winter, the chemistry plays a minor role, and high daytime emissions dominate the diurnal variation in NO2, balanced by transport. In summer, emissions, chemistry, and transport play an important role in shaping the diurnal variation in NO2.
M. Omar Nawaz, Jeremiah Johnson, Greg Yarwood, Benjamin de Foy, Laura Judd, and Daniel L. Goldberg
Atmos. Chem. Phys., 24, 6719–6741, https://doi.org/10.5194/acp-24-6719-2024, https://doi.org/10.5194/acp-24-6719-2024, 2024
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NO2 is a gas with implications for air pollution. A campaign conducted in Houston provided an opportunity to compare NO2 from different instruments and a model. Aircraft and satellite observations agreed well with measurements on the ground; however, the latter estimated lower values. We find that model-simulated NO2 was lower than observations, especially downtown, suggesting that NO2 sources associated with the urban core of Houston, such as vehicle emissions, may be underestimated.
Natalie Brett, Kathy S. Law, Steve R. Arnold, Javier G. Fochesatto, Jean-Christophe Raut, Tatsuo Onishi, Robert Gilliam, Kathleen Fahey, Deanna Huff, George Pouliot, Brice Barret, Elsa Dieudonne, Roman Pohorsky, Julia Schmale, Andrea Baccarini, Slimane Bekki, Gianluca Pappaccogli, Federico Scoto, Stefano Decesari, Antonio Donateo, Meeta Cesler-Maloney, William Simpson, Patrice Medina, Barbara D'Anna, Brice Temime-Roussel, Joel Savarino, Sarah Albertin, Jingqiu Mao, Becky Alexander, Allison Moon, Peter F. DeCarlo, Vanessa Selimovic, Robert Yokelson, and Ellis S. Robinson
EGUsphere, https://doi.org/10.5194/egusphere-2024-1450, https://doi.org/10.5194/egusphere-2024-1450, 2024
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Processes influencing dispersion of local anthropogenic emissions in Arctic wintertime are investigated with dispersion model simulations. Modelled power plant plume rise that considers surface and elevated temperature inversions improves results compared to observations. Modelled near-surface concentrations are improved by representation of vertical mixing and emission estimates. Large increases in diesel vehicle emissions at temperatures reaching -35 °C are required to reproduce observed NOx.
Tianlang Zhao, Jingqiu Mao, Zolal Ayazpour, Gonzalo González Abad, Caroline R. Nowlan, and Yiqi Zheng
Atmos. Chem. Phys., 24, 6105–6121, https://doi.org/10.5194/acp-24-6105-2024, https://doi.org/10.5194/acp-24-6105-2024, 2024
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HCHO variability is a key tracer in understanding VOC emissions in response to climate change. We investigate the role of methane oxidation and biogenic and wildfire emissions in HCHO interannual variability over northern high latitudes in summer, emphasizing wildfires as a key driver of HCHO interannual variability in Alaska, Siberia and northern Canada using satellite HCHO and SIF retrievals and then GEOS-Chem model. We show SIF is a tool to understand biogenic HCHO variability in this region.
Jianghao Li, Alastair C. Lewis, Jim R. Hopkins, Stephen J. Andrews, Tim Murrells, Neil Passant, Ben Richmond, Siqi Hou, William J. Bloss, Roy M. Harrison, and Zongbo Shi
Atmos. Chem. Phys., 24, 6219–6231, https://doi.org/10.5194/acp-24-6219-2024, https://doi.org/10.5194/acp-24-6219-2024, 2024
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A summertime ozone event at an urban site in Birmingham is sensitive to volatile organic compounds (VOCs) – particularly those of oxygenated VOCs. The roles of anthropogenic VOC sources in urban ozone chemistry are examined by integrating the 1990–2019 national atmospheric emission inventory into model scenarios. Road transport remains the most powerful means of further reducing ozone in this case study, but the benefits may be offset if solvent emissions of VOCs continue to increase.
Kai-Lan Chang, Owen R. Cooper, Audrey Gaudel, Irina Petropavlovskikh, Peter Effertz, Gary Morris, and Brian C. McDonald
Atmos. Chem. Phys., 24, 6197–6218, https://doi.org/10.5194/acp-24-6197-2024, https://doi.org/10.5194/acp-24-6197-2024, 2024
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A great majority of observational trend studies of free tropospheric ozone use sparsely sampled ozonesonde and aircraft measurements as reference data sets. A ubiquitous assumption is that trends are accurate and reliable so long as long-term records are available. We show that sampling bias due to sparse samples can persistently reduce the trend accuracy, and we highlight the importance of maintaining adequate frequency and continuity of observations.
Jin Ma, Linda M. J. Kooijmans, Norbert Glatthor, Stephen A. Montzka, Marc von Hobe, Thomas Röckmann, and Maarten C. Krol
Atmos. Chem. Phys., 24, 6047–6070, https://doi.org/10.5194/acp-24-6047-2024, https://doi.org/10.5194/acp-24-6047-2024, 2024
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The global budget of atmospheric COS can be optimised by inverse modelling using TM5-4DVAR, with the co-constraints of NOAA surface observations and MIPAS satellite data. We found reduced COS biosphere uptake from inversions and improved land and ocean separation using MIPAS satellite data assimilation. Further improvements are expected from better quantification of COS ocean and biosphere fluxes.
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Short summary
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.
Methane (CH4) is an important greenhouse gas. The growth of atmospheric CH4 stalled from 1999 to...
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