Articles | Volume 14, issue 2
https://doi.org/10.5194/acp-14-979-2014
© Author(s) 2014. 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-14-979-2014
© Author(s) 2014. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
28 Jan 2014
Research article |
| 28 Jan 2014
Estimates of tropical bromoform emissions using an inversion method
M. J. Ashfold
Department of Chemistry, University of Cambridge, Cambridge, UK
now at: School of Biosciences, University of Nottingham Malaysia Campus, Jalan Broga, 43500 Semenyih, Selangor Darul Ehsan, Malaysia
N. R. P. Harris
Department of Chemistry, University of Cambridge, Cambridge, UK
A. J. Manning
Met Office, Exeter, UK
A. D. Robinson
Department of Chemistry, University of Cambridge, Cambridge, UK
N. J. Warwick
Department of Chemistry, University of Cambridge, Cambridge, UK
National Centre for Atmospheric Science, UK
J. A. Pyle
Department of Chemistry, University of Cambridge, Cambridge, UK
National Centre for Atmospheric Science, UK
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Alice E. Ramsden, Anita L. Ganesan, Luke M. Western, Matthew Rigby, Alistair J. Manning, Amy Foulds, James L. France, Patrick Barker, Peter Levy, Daniel Say, Adam Wisher, Tim Arnold, Chris Rennick, Kieran M. Stanley, Dickon Young, and Simon O'Doherty
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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.
Eric Saboya, Giulia Zazzeri, Heather Graven, Alistair J. Manning, and Sylvia Englund Michel
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Sebastian Landwehr, Michele Volpi, F. Alexander Haumann, Charlotte M. Robinson, Iris Thurnherr, Valerio Ferracci, Andrea Baccarini, Jenny Thomas, Irina Gorodetskaya, Christian Tatzelt, Silvia Henning, Rob L. Modini, Heather J. Forrer, Yajuan Lin, Nicolas Cassar, Rafel Simó, Christel Hassler, Alireza Moallemi, Sarah E. Fawcett, Neil Harris, Ruth Airs, Marzieh H. Derkani, Alberto Alberello, Alessandro Toffoli, Gang Chen, Pablo Rodríguez-Ros, Marina Zamanillo, Pau Cortés-Greus, Lei Xue, Conor G. Bolas, Katherine C. Leonard, Fernando Perez-Cruz, David Walton, and Julia Schmale
Earth Syst. Dynam., 12, 1295–1369, https://doi.org/10.5194/esd-12-1295-2021, https://doi.org/10.5194/esd-12-1295-2021, 2021
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The Antarctic Circumnavigation Expedition surveyed a large number of variables describing the dynamic state of ocean and atmosphere, freshwater cycle, atmospheric chemistry, ocean biogeochemistry, and microbiology in the Southern Ocean. To reduce the dimensionality of the dataset, we apply a sparse principal component analysis and identify temporal patterns from diurnal to seasonal cycles, as well as geographical gradients and
hotspotsof interaction. Code and data are open access.
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.
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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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.
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.
James L. France, Prudence Bateson, Pamela Dominutti, Grant Allen, Stephen Andrews, Stephane Bauguitte, Max Coleman, Tom Lachlan-Cope, Rebecca E. Fisher, Langwen Huang, Anna E. Jones, James Lee, David Lowry, Joseph Pitt, Ruth Purvis, John Pyle, Jacob Shaw, Nicola Warwick, Alexandra Weiss, Shona Wilde, Jonathan Witherstone, and Stuart Young
Atmos. Meas. Tech., 14, 71–88, https://doi.org/10.5194/amt-14-71-2021, https://doi.org/10.5194/amt-14-71-2021, 2021
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Measuring emission rates of methane from installations is tricky, and it is even more so when those installations are located offshore. Here, we show the aircraft set-up and demonstrate an effective methodology for surveying emissions from UK and Dutch offshore oil and gas installations. We present example data collected from two campaigns to demonstrate the challenges and solutions encountered during these surveys.
Peter G. Simmonds, Matthew Rigby, Alistair J. Manning, Sunyoung Park, Kieran M. Stanley, Archie McCulloch, Stephan Henne, Francesco Graziosi, Michela Maione, Jgor Arduini, Stefan Reimann, Martin K. Vollmer, Jens Mühle, Simon O'Doherty, Dickon Young, Paul B. Krummel, Paul J. Fraser, Ray F. Weiss, Peter K. Salameh, Christina M. Harth, Mi-Kyung Park, Hyeri Park, Tim Arnold, Chris Rennick, L. Paul Steele, Blagoj Mitrevski, Ray H. J. Wang, and Ronald G. Prinn
Atmos. Chem. Phys., 20, 7271–7290, https://doi.org/10.5194/acp-20-7271-2020, https://doi.org/10.5194/acp-20-7271-2020, 2020
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Sulfur hexafluoride (SF6) is a potent greenhouse gas which is regulated under the Kyoto Protocol. From a 40-year record of measurements, collected at five global monitoring sites and archived air samples, we show that its concentration in the atmosphere has steadily increased. Using modelling techniques, we estimate that global emissions have increased by about 24 % over the past decade. We find that this increase is driven by the demand for SF6-insulated switchgear in developing countries.
Luke M. Western, Zhe Sha, Matthew Rigby, Anita L. Ganesan, Alistair J. Manning, Kieran M. Stanley, Simon J. O'Doherty, Dickon Young, and Jonathan Rougier
Geosci. Model Dev., 13, 2095–2107, https://doi.org/10.5194/gmd-13-2095-2020, https://doi.org/10.5194/gmd-13-2095-2020, 2020
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Assessments of greenhouse gas emissions using atmospheric measurements and meteorological models, or
top-downmethods, are important to verify national inventories or produce a stand-alone estimate where no inventory exists. We present a novel top-down method to estimate emissions. This approach uses a fast method called an integrated nested Laplacian approximation to estimate how these emissions are correlated with other emissions in different locations and at different times.
Elise S. Droste, Karina E. Adcock, Matthew J. Ashfold, Charles Chou, Zoë Fleming, Paul J. Fraser, Lauren J. Gooch, Andrew J. Hind, Ray L. Langenfelds, Emma C. Leedham Elvidge, Norfazrin Mohd Hanif, Simon O'Doherty, David E. Oram, Chang-Feng Ou-Yang, Marios Panagi, Claire E. Reeves, William T. Sturges, and Johannes C. Laube
Atmos. Chem. Phys., 20, 4787–4807, https://doi.org/10.5194/acp-20-4787-2020, https://doi.org/10.5194/acp-20-4787-2020, 2020
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We update the tropospheric trends and emissions of six perfluorocarbon (PFC) gases, including separate isomers. Trends for these strong greenhouse gases are still increasing, but at slower rates than previously. The lack of natural sinks results in the global accumulation of 833 million metric tonnes of CO2 equivalent for these six PFCs by 2017. Modelling results indicate potential source regions and types in East Asia, but we find that many emissions are unaccounted for in emission reports.
Marios Panagi, Zoë L. Fleming, Paul S. Monks, Matthew J. Ashfold, Oliver Wild, Michael Hollaway, Qiang Zhang, Freya A. Squires, and Joshua D. Vande Hey
Atmos. Chem. Phys., 20, 2825–2838, https://doi.org/10.5194/acp-20-2825-2020, https://doi.org/10.5194/acp-20-2825-2020, 2020
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In this paper, using dispersion modelling with emission inventories it was determined that on average 45 % of the total CO pollution that affects Beijing is transported from other areas. About half of the CO comes from beyond the immediate surrounding areas. Finally three classification types of pollution were identified and used to analyse the APHH winter campaign. The results can inform targeted control measures to be implemented in Beijing and the other regions to tackle air quality problems.
Conor G. Bolas, Valerio Ferracci, Andrew D. Robinson, Mohammed I. Mead, Mohd Shahrul Mohd Nadzir, John A. Pyle, Roderic L. Jones, and Neil R. P. Harris
Atmos. Meas. Tech., 13, 821–838, https://doi.org/10.5194/amt-13-821-2020, https://doi.org/10.5194/amt-13-821-2020, 2020
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Here we present the iDirac, a new instrument capable of making isoprene measurements in remote and challenging environments. The iDirac is a customisable and rugged field instrument for investigating emissions of volatile organic compounds from vegetation. It has been tested here in a series of experiments to ensure a high degree of technical precision, accuracy and repeatability. This new instrument allows us to ask and answer new questions about the influence of vegetation on the atmosphere.
Michal T. Filus, Elliot L. Atlas, Maria A. Navarro, Elena Meneguz, David Thomson, Matthew J. Ashfold, Lucy J. Carpenter, Stephen J. Andrews, and Neil R. P. Harris
Atmos. Chem. Phys., 20, 1163–1181, https://doi.org/10.5194/acp-20-1163-2020, https://doi.org/10.5194/acp-20-1163-2020, 2020
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The effectiveness of transport of short-lived halocarbons to the upper troposphere and lower stratosphere remains an important unknown in quantifying the supply of ozone-depleting substances to the stratosphere. In early 2014, a major field campaign in Guam in the western Pacific, involving UK and US research aircraft, sampled the tropical troposphere and lower stratosphere. The resulting measurements of CH3I, CHBr3 and CH2Br2 are compared here with calculations from a Lagrangian model.
Kuo-Ying Wang, Philippe Nedelec, Hannah Clark, and Neil Harris
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2019-156, https://doi.org/10.5194/essd-2019-156, 2019
Revised manuscript not accepted
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Atmospheric dispersion of radioactive materials following the accidents of the 11 March 2011 Fukushima Nuclear Power Plants contain very distinctive characteristics
over the land surface areas and over the oceanic atmosphere. Air dose rates measured over the land surface areas exhibit a combination of the effects from the deposited radioactive materials on the surface and the airborne radioactive materials. Air dose rates measured over the oceanic atmosphere were due to airborne particles.
Ann R. Stavert, Simon O'Doherty, Kieran Stanley, Dickon Young, Alistair J. Manning, Mark F. Lunt, Christopher Rennick, and Tim Arnold
Atmos. Meas. Tech., 12, 4495–4518, https://doi.org/10.5194/amt-12-4495-2019, https://doi.org/10.5194/amt-12-4495-2019, 2019
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Under the UK GAUGE project, two new greenhouse gas observation sites were established in the 2013/2014 winter at two telecommunications towers. A combination of spectroscopic and chromatographic instrumentation was used to measure CO2, CH4, CO, N2O and SF6. The advantages and disadvantages of two CRDS sample drying strategies, Nafion(R) and empirical water correction, were also examined.
Jens Mühle, Cathy M. Trudinger, Luke M. Western, Matthew Rigby, Martin K. Vollmer, Sunyoung Park, Alistair J. Manning, Daniel Say, Anita Ganesan, L. Paul Steele, Diane J. Ivy, Tim Arnold, Shanlan Li, Andreas Stohl, Christina M. Harth, Peter K. Salameh, Archie McCulloch, Simon O'Doherty, Mi-Kyung Park, Chun Ok Jo, Dickon Young, Kieran M. Stanley, Paul B. Krummel, Blagoj Mitrevski, Ove Hermansen, Chris Lunder, Nikolaos Evangeliou, Bo Yao, Jooil Kim, Benjamin Hmiel, Christo Buizert, Vasilii V. Petrenko, Jgor Arduini, Michela Maione, David M. Etheridge, Eleni Michalopoulou, Mike Czerniak, Jeffrey P. Severinghaus, Stefan Reimann, Peter G. Simmonds, Paul J. Fraser, Ronald G. Prinn, and Ray F. Weiss
Atmos. Chem. Phys., 19, 10335–10359, https://doi.org/10.5194/acp-19-10335-2019, https://doi.org/10.5194/acp-19-10335-2019, 2019
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We discuss atmospheric concentrations and emissions of the strong greenhouse gas perfluorocyclobutane. A large fraction of recent emissions stem from China, India, and Russia, probably as a by-product from the production of fluoropolymers and fluorochemicals. Most historic emissions likely stem from developed countries. Total emissions are higher than what is being reported. Clearly, more measurements and better reporting are needed to understand emissions of this and other greenhouse gases.
Daniel Say, Anita L. Ganesan, Mark F. Lunt, Matthew Rigby, Simon O'Doherty, Christina Harth, Alistair J. Manning, Paul B. Krummel, and Stephane Bauguitte
Atmos. Chem. Phys., 19, 9865–9885, https://doi.org/10.5194/acp-19-9865-2019, https://doi.org/10.5194/acp-19-9865-2019, 2019
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Despite its emergence as a global economic power, very little information exists regarding India's halocarbon (CFC, HCFC, HFC and chlorocarbon) emissions. We report atmospheric measurements of these gases from above India, and use them to estimate India's emissions. Our results are consistent with the emissions profile of a developing country, with large emissions of HCFCs, HFCs and chlorocarbons not regulated under the Montreal Protocol, but little evidence for ongoing CFC consumption.
Stuart N. Riddick, Denise L. Mauzerall, Michael Celia, Neil R. P. Harris, Grant Allen, Joseph Pitt, John Staunton-Sykes, Grant L. Forster, Mary Kang, David Lowry, Euan G. Nisbet, and Alistair J. Manning
Atmos. Chem. Phys., 19, 9787–9796, https://doi.org/10.5194/acp-19-9787-2019, https://doi.org/10.5194/acp-19-9787-2019, 2019
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Currently, bottom-up methods estimate that 0.13 % of methane produced by UK North Sea oil and gas installations is lost. Here we measure emissions from eight platforms in the North Sea and, when considered collectively, the methane loss is estimated at 0.19 % of gas production. As this ambient loss is not explicitly accounted for in the bottom-up approach, these measured emissions represent significant additional emissions above previous estimates.
Joseph R. Pitt, Grant Allen, Stéphane J.-B. Bauguitte, Martin W. Gallagher, James D. Lee, Will Drysdale, Beth Nelson, Alistair J. Manning, and Paul I. Palmer
Atmos. Chem. Phys., 19, 8931–8945, https://doi.org/10.5194/acp-19-8931-2019, https://doi.org/10.5194/acp-19-8931-2019, 2019
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This paper presents a new method to assess inventory estimates of greenhouse gas and air pollutant emissions for large cities and their surrounding regions. A case study using data sampled by a research aircraft around London was used to test the method. We found that the UK national inventory agrees with our observations for CO but needed lower emissions for CH4 to agree with the measured data. Repeated studies could help determine how these emissions vary on different timescales.
Emily D. White, Matthew Rigby, Mark F. Lunt, T. Luke Smallman, Edward Comyn-Platt, Alistair J. Manning, Anita L. Ganesan, Simon O'Doherty, Ann R. Stavert, Kieran Stanley, Mathew Williams, Peter Levy, Michel Ramonet, Grant L. Forster, Andrew C. Manning, and Paul I. Palmer
Atmos. Chem. Phys., 19, 4345–4365, https://doi.org/10.5194/acp-19-4345-2019, https://doi.org/10.5194/acp-19-4345-2019, 2019
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Understanding carbon dioxide (CO2) fluxes from the terrestrial biosphere on a national scale is important for evaluating land use strategies to mitigate climate change. We estimate emissions of CO2 from the UK biosphere using atmospheric data in a top-down approach. Our findings show that bottom-up estimates from models of biospheric fluxes overestimate the amount of CO2 uptake in summer. This suggests these models wrongly estimate or omit key processes, e.g. land disturbance due to harvest.
Kieran Brophy, Heather Graven, Alistair J. Manning, Emily White, Tim Arnold, Marc L. Fischer, Seongeun Jeong, Xinguang Cui, and Matthew Rigby
Atmos. Chem. Phys., 19, 2991–3006, https://doi.org/10.5194/acp-19-2991-2019, https://doi.org/10.5194/acp-19-2991-2019, 2019
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We investigate potential errors and uncertainties related to the spatial and temporal prior representation of emissions and modelled atmospheric transport for the inversion of California's fossil fuel CO2 emissions. Our results indicate that uncertainties in posterior total state fossil fuel CO2 estimates arising from the choice of prior emissions or atmospheric transport model are on the order of 15 % or less for the ground-based network in California we consider.
Daniel Say, Anita L. Ganesan, Mark F. Lunt, Matthew Rigby, Simon O'Doherty, Chris Harth, Alistair J. Manning, Paul B. Krummel, and Stephane Bauguitte
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-1287, https://doi.org/10.5194/acp-2018-1287, 2019
Publication in ACP not foreseen
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India is a potentially significant source of chlorocarbons, gases typically used as solvents and feedstocks. Given the potential for these species to deplete stratospheric ozone, understanding their sources is important. We use flask measurements collected from an aircraft to infer India's chlorocarbon emissions. We link emissions of carbon tetrachloride to the industrial production of other chloromethanes, and provide evidence for rapid growth in India's emissions of dichloromethane.
Sarah Connors, Alistair J. Manning, Andrew D. Robinson, Stuart N. Riddick, Grant L. Forster, Anita Ganesan, Aoife Grant, Stephen Humphrey, Simon O'Doherty, Dave E. Oram, Paul I. Palmer, Robert L. Skelton, Kieran Stanley, Ann Stavert, Dickon Young, and Neil R. P. Harris
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-1187, https://doi.org/10.5194/acp-2018-1187, 2018
Preprint withdrawn
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Methane is an important greenhouse gas & reducing its emissions is a vital part of climate change mitigation to limit global temperature increase to 1.5 °C or 2.0 °C. This paper explains a way to estimate emitted methane over a sub-national area by combining measurements & computer dispersion modelling in a so-called
inversiontechnique. Compared with the current national inventory, our results show lower emissions for Cambridgeshire, possibly due to waste sector emission differences.
Liang Feng, Paul I. Palmer, Robyn Butler, Stephen J. Andrews, Elliot L. Atlas, Lucy J. Carpenter, Valeria Donets, Neil R. P. Harris, Ross J. Salawitch, Laura L. Pan, and Sue M. Schauffler
Atmos. Chem. Phys., 18, 14787–14798, https://doi.org/10.5194/acp-18-14787-2018, https://doi.org/10.5194/acp-18-14787-2018, 2018
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We infer surface fluxes of bromoform (CHBr3) and dibromoform (CH2Br2) from CAST and CONTRAST aircraft observations over the western Pacific, using a tagged version of the GEOS-Chem global 3-D atmospheric chemistry model and a Maximum A Posteriori inverse model. Using the aircraft data, we estimate the regional fluxes about 20–40 % smaller than the prior inventories by Ordóñez et al. (2012). We find no evidence to support a robust linear relationship between CHBr3 and CH2Br2 oceanic emissions.
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.
James Keeble, Hannah Brown, N. Luke Abraham, Neil R. P. Harris, and John A. Pyle
Atmos. Chem. Phys., 18, 7625–7637, https://doi.org/10.5194/acp-18-7625-2018, https://doi.org/10.5194/acp-18-7625-2018, 2018
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2017 marks the 30th anniversary of the Montreal Protocol, which was implemented to protect the stratospheric ozone layer from the harmful effects of synthetic ozone depleting substances. Since the late 1990s atmospheric concentrations of these species have begun to decline, and as a result ozone concentrations are expected to increase. In this study we use an ensemble of chemistry–climate simulations to investigate recent ozone trends and search for early signs of ozone recovery.
Karina E. Adcock, Claire E. Reeves, Lauren J. Gooch, Emma C. Leedham Elvidge, Matthew J. Ashfold, Carl A. M. Brenninkmeijer, Charles Chou, Paul J. Fraser, Ray L. Langenfelds, Norfazrin Mohd Hanif, Simon O'Doherty, David E. Oram, Chang-Feng Ou-Yang, Siew Moi Phang, Azizan Abu Samah, Thomas Röckmann, William T. Sturges, and Johannes C. Laube
Atmos. Chem. Phys., 18, 4737–4751, https://doi.org/10.5194/acp-18-4737-2018, https://doi.org/10.5194/acp-18-4737-2018, 2018
Peter G. Simmonds, Matthew Rigby, Archie McCulloch, Martin K. Vollmer, Stephan Henne, Jens Mühle, Simon O'Doherty, Alistair J. Manning, Paul B. Krummel, Paul J. Fraser, Dickon Young, Ray F. Weiss, Peter K. Salameh, Christina M. Harth, Stefan Reimann, Cathy M. Trudinger, L. Paul Steele, Ray H. J. Wang, Diane J. Ivy, Ronald G. Prinn, Blagoj Mitrevski, and David M. Etheridge
Atmos. Chem. Phys., 18, 4153–4169, https://doi.org/10.5194/acp-18-4153-2018, https://doi.org/10.5194/acp-18-4153-2018, 2018
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Recent measurements of the potent greenhouse gas HFC-23, a by-product of HCFC-22 production, show a 28 % increase in the atmospheric mole fraction from 2009 to 2016. A minimum in the atmospheric abundance of HFC-23 in 2009 was attributed to abatement of HFC-23 emissions by incineration under the Clean Development Mechanism (CDM). Our results indicate that the recent increase in HFC-23 emissions is driven by failure of mitigation under the CDM to keep pace with increased HCFC-22 production.
Kieran M. Stanley, Aoife Grant, Simon O'Doherty, Dickon Young, Alistair J. Manning, Ann R. Stavert, T. Gerard Spain, Peter K. Salameh, Christina M. Harth, Peter G. Simmonds, William T. Sturges, David E. Oram, and Richard G. Derwent
Atmos. Meas. Tech., 11, 1437–1458, https://doi.org/10.5194/amt-11-1437-2018, https://doi.org/10.5194/amt-11-1437-2018, 2018
Peter Bergamaschi, Ute Karstens, Alistair J. Manning, Marielle Saunois, Aki Tsuruta, Antoine Berchet, Alexander T. Vermeulen, Tim Arnold, Greet Janssens-Maenhout, Samuel Hammer, Ingeborg Levin, Martina Schmidt, Michel Ramonet, Morgan Lopez, Jost Lavric, Tuula Aalto, Huilin Chen, Dietrich G. Feist, Christoph Gerbig, László Haszpra, Ove Hermansen, Giovanni Manca, John Moncrieff, Frank Meinhardt, Jaroslaw Necki, Michal Galkowski, Simon O'Doherty, Nina Paramonova, Hubertus A. Scheeren, Martin Steinbacher, and Ed Dlugokencky
Atmos. Chem. Phys., 18, 901–920, https://doi.org/10.5194/acp-18-901-2018, https://doi.org/10.5194/acp-18-901-2018, 2018
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European methane (CH4) emissions are estimated for 2006–2012 using atmospheric in situ measurements from 18 European monitoring stations and 7 different inverse models. Our analysis highlights the potential significant contribution of natural emissions from wetlands (including peatlands and wet soils) to the total European emissions. The top-down estimates of total EU-28 CH4 emissions are broadly consistent with the sum of reported anthropogenic CH4 emissions and the estimated natural emissions.
James Keeble, Ewa M. Bednarz, Antara Banerjee, N. Luke Abraham, Neil R. P. Harris, Amanda C. Maycock, and John A. Pyle
Atmos. Chem. Phys., 17, 13801–13818, https://doi.org/10.5194/acp-17-13801-2017, https://doi.org/10.5194/acp-17-13801-2017, 2017
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In this study we explore the chemical and transport processes controlling ozone abundances in different altitude regions in the tropics for the present day and how these processes may change in the future in order to determine when total-column ozone values in the tropics will recover to pre-1980s values following the implementation of the Montreal Protocol and its subsequent amendments, which imposed bans on the use and emissions of CFCs.
Hannah Sonderfeld, Hartmut Bösch, Antoine P. R. Jeanjean, Stuart N. Riddick, Grant Allen, Sébastien Ars, Stewart Davies, Neil Harris, Neil Humpage, Roland Leigh, and Joseph Pitt
Atmos. Meas. Tech., 10, 3931–3946, https://doi.org/10.5194/amt-10-3931-2017, https://doi.org/10.5194/amt-10-3931-2017, 2017
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The waste sector is the second largest source of methane in the UK. However, uncertainties of methane emissions from landfill sites still remain. In this study we present a new approach for the estimation of methane emissions from a landfill site by applying a computational fluid dynamics (CFD) model for precise measurements of methane with in situ Fourier-transform infrared (FTIR) spectroscopy. Different source areas could be distinguished with this method and their emissions were assessed.
David E. Oram, Matthew J. Ashfold, Johannes C. Laube, Lauren J. Gooch, Stephen Humphrey, William T. Sturges, Emma C. Leedham Elvidge, Grant L. Forster, Neil R. P. Harris, Mohammed Iqbal Mead, Azizan Abu Samah, Siew Moi Phang, Chang-Feng Ou-Yang, Neng-Huei Lin, Jia-Lin Wang, Angela K. Baker, Carl A. M. Brenninkmeijer, and David Sherry
Atmos. Chem. Phys., 17, 11929–11941, https://doi.org/10.5194/acp-17-11929-2017, https://doi.org/10.5194/acp-17-11929-2017, 2017
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We have observed large amounts of man-made chlorine compounds in E and SE Asia and in the upper tropical troposphere. These relatively short-lived compounds are not controlled by the Montreal Protocol, but if significant quantities were able to reach the stratosphere, the long-term recovery of stratospheric ozone would be delayed. We have also identified an important atmospheric transport mechanism that can rapidly transport these chemicals from E Asia to the upper troposphere via the tropics.
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.
Wolfgang Steinbrecht, Lucien Froidevaux, Ryan Fuller, Ray Wang, John Anderson, Chris Roth, Adam Bourassa, Doug Degenstein, Robert Damadeo, Joe Zawodny, Stacey Frith, Richard McPeters, Pawan Bhartia, Jeannette Wild, Craig Long, Sean Davis, Karen Rosenlof, Viktoria Sofieva, Kaley Walker, Nabiz Rahpoe, Alexei Rozanov, Mark Weber, Alexandra Laeng, Thomas von Clarmann, Gabriele Stiller, Natalya Kramarova, Sophie Godin-Beekmann, Thierry Leblanc, Richard Querel, Daan Swart, Ian Boyd, Klemens Hocke, Niklaus Kämpfer, Eliane Maillard Barras, Lorena Moreira, Gerald Nedoluha, Corinne Vigouroux, Thomas Blumenstock, Matthias Schneider, Omaira García, Nicholas Jones, Emmanuel Mahieu, Dan Smale, Michael Kotkamp, John Robinson, Irina Petropavlovskikh, Neil Harris, Birgit Hassler, Daan Hubert, and Fiona Tummon
Atmos. Chem. Phys., 17, 10675–10690, https://doi.org/10.5194/acp-17-10675-2017, https://doi.org/10.5194/acp-17-10675-2017, 2017
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Thanks to the 1987 Montreal Protocol and its amendments, ozone-depleting chlorine (and bromine) in the stratosphere has declined slowly since the late 1990s. Improved and extended long-term ozone profile observations from satellites and ground-based stations confirm that ozone is responding as expected and has increased by about 2 % per decade since 2000 in the upper stratosphere, around 40 km altitude. At lower altitudes, however, ozone has not changed significantly since 2000.
Stuart N. Riddick, Sarah Connors, Andrew D. Robinson, Alistair J. Manning, Pippa S. D. Jones, David Lowry, Euan Nisbet, Robert L. Skelton, Grant Allen, Joseph Pitt, and Neil R. P. Harris
Atmos. Chem. Phys., 17, 7839–7851, https://doi.org/10.5194/acp-17-7839-2017, https://doi.org/10.5194/acp-17-7839-2017, 2017
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High methane mixing ratios occurred at our long-term measurement site. Isotopic measurements show the source is a landfill 7 km away; the emissions were estimated using three different approaches. The emission estimates made by near-source and middle-distance methods agree well for a period of intense observation. The estimate of the inverse modelling is similar to the labour-intensive middle-distance approach, which shows it can be used to identify point sources within an emission landscape.
Peter G. Simmonds, Matthew Rigby, Archie McCulloch, Simon O'Doherty, Dickon Young, Jens Mühle, Paul B. Krummel, Paul Steele, Paul J. Fraser, Alistair J. Manning, Ray F. Weiss, Peter K. Salameh, Chris M. Harth, Ray H. J. Wang, and Ronald G. Prinn
Atmos. Chem. Phys., 17, 4641–4655, https://doi.org/10.5194/acp-17-4641-2017, https://doi.org/10.5194/acp-17-4641-2017, 2017
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This paper reports how long-term atmospheric measurements demonstrate that the Montreal Protocol has been effective in controlling production and consumption of the hydrochlorofluorocarbons, a group of industrial chemicals that have detrimental effects on the ozone layer and also contribute to global warming as greenhouse gases and their hydrofluorocarbon substitutes which are also potent greenhouse gases but do not materially affect the ozone layer.
Nicola J. Warwick, Michelle L. Cain, Rebecca Fisher, James L. France, David Lowry, Sylvia E. Michel, Euan G. Nisbet, Bruce H. Vaughn, James W. C. White, and John A. Pyle
Atmos. Chem. Phys., 16, 14891–14908, https://doi.org/10.5194/acp-16-14891-2016, https://doi.org/10.5194/acp-16-14891-2016, 2016
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Methane is an important greenhouse gas. Methane emissions from Arctic wetlands are poorly quantified and may increase in a warming climate. Using a global atmospheric model and atmospheric observations of methane and its isotopologues, we find that isotopologue data are useful in constraining Arctic wetland emissions. Our results suggest that the seasonal cycle of these emissions may be incorrectly simulated in land process models, with implications for our understanding of future emissions.
Francesco Graziosi, Jgor Arduini, Paolo Bonasoni, Francesco Furlani, Umberto Giostra, Alistair J. Manning, Archie McCulloch, Simon O'Doherty, Peter G. Simmonds, Stefan Reimann, Martin K. Vollmer, and Michela Maione
Atmos. Chem. Phys., 16, 12849–12859, https://doi.org/10.5194/acp-16-12849-2016, https://doi.org/10.5194/acp-16-12849-2016, 2016
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Carbon tetrachloride is an ozone-depleting greenhouse gas banned under the Montreal Protocol. Measurements of atmospheric levels combined with global transport models indicate that it is still being emitted, in contrast to what is reported. In order to help solve the "mystery of carbon tetrachloride", we estimated European emissions during 2006–2014 using atmospheric observations and models. We identified emission hot spots and showed inconsistencies in national emission declarations.
Mark F. Lunt, Matt Rigby, Anita L. Ganesan, and Alistair J. Manning
Geosci. Model Dev., 9, 3213–3229, https://doi.org/10.5194/gmd-9-3213-2016, https://doi.org/10.5194/gmd-9-3213-2016, 2016
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Bayesian inversions can be used to estimate emissions of gases from atmospheric data. We present an inversion framework that objectively defines the basis functions, which describe regions of emissions. The framework allows for the uncertainty in the choice of basis functions to be propagated through to the posterior emissions distribution in a single-step process, and provides an alternative to using a single set of basis functions.
P. G. Simmonds, M. Rigby, A. J. Manning, M. F. Lunt, S. O'Doherty, A. McCulloch, P. J. Fraser, S. Henne, M. K. Vollmer, J. Mühle, R. F. Weiss, P. K. Salameh, D. Young, S. Reimann, A. Wenger, T. Arnold, C. M. Harth, P. B. Krummel, L. P. Steele, B. L. Dunse, B. R. Miller, C. R. Lunder, O. Hermansen, N. Schmidbauer, T. Saito, Y. Yokouchi, S. Park, S. Li, B. Yao, L. X. Zhou, J. Arduini, M. Maione, R. H. J. Wang, D. Ivy, and R. G. Prinn
Atmos. Chem. Phys., 16, 365–382, https://doi.org/10.5194/acp-16-365-2016, https://doi.org/10.5194/acp-16-365-2016, 2016
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We report regional and global emissions estimates of HFC-152a using high frequency measurements from 11 observing sites and archived air samples dating back to 1978 together with atmospheric transport models. The "bottom-up" emissions of HFC-152a reported to the UNFCCC appear to significantly underestimate those reported here from observations. This discrepancy we suggest arises from largely underestimated USA and undeclared Asian emissions.
M. R. Russo, M. J. Ashfold, N. R. P. Harris, and J. A. Pyle
Atmos. Chem. Phys., 15, 14031–14040, https://doi.org/10.5194/acp-15-14031-2015, https://doi.org/10.5194/acp-15-14031-2015, 2015
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We find a strong regional element to the uplift of CHBr3 from the ocean to the upper troposphere and lower stratosphere. The strongest uplift occurs when the largest emission and the most intense convection are co-located which is over the Maritime Continent in northern winter. Estimates of CHBr3 emissions based on aircraft measurements will be sensitive to where the available aircraft campaigns took place.
R. S. Humphries, R. Schofield, M. D. Keywood, J. Ward, J. R. Pierce, C. M. Gionfriddo, M. T. Tate, D. P. Krabbenhoft, I. E. Galbally, S. B. Molloy, A. R. Klekociuk, P. V. Johnston, K. Kreher, A. J. Thomas, A. D. Robinson, N. R. P. Harris, R. Johnson, and S. R. Wilson
Atmos. Chem. Phys., 15, 13339–13364, https://doi.org/10.5194/acp-15-13339-2015, https://doi.org/10.5194/acp-15-13339-2015, 2015
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An atmospheric new particle formation event that was observed in the pristine East Antarctic pack ice during a springtime voyage in 2012 is characterised in terms of formation and growth rates. Known nucleation mechanisms (e.g. those involving sulfate, iodine and organics) were unable to explain observations; however, correlations with total gaseous mercury were found, leading to the suggestion of a possible mercury-driven nucleation mechanism not previously described.
N. R. P. Harris, B. Hassler, F. Tummon, G. E. Bodeker, D. Hubert, I. Petropavlovskikh, W. Steinbrecht, J. Anderson, P. K. Bhartia, C. D. Boone, A. Bourassa, S. M. Davis, D. Degenstein, A. Delcloo, S. M. Frith, L. Froidevaux, S. Godin-Beekmann, N. Jones, M. J. Kurylo, E. Kyrölä, M. Laine, S. T. Leblanc, J.-C. Lambert, B. Liley, E. Mahieu, A. Maycock, M. de Mazière, A. Parrish, R. Querel, K. H. Rosenlof, C. Roth, C. Sioris, J. Staehelin, R. S. Stolarski, R. Stübi, J. Tamminen, C. Vigouroux, K. A. Walker, H. J. Wang, J. Wild, and J. M. Zawodny
Atmos. Chem. Phys., 15, 9965–9982, https://doi.org/10.5194/acp-15-9965-2015, https://doi.org/10.5194/acp-15-9965-2015, 2015
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Trends in the vertical distribution of ozone are reported for new and recently revised data sets. The amount of ozone-depleting compounds in the stratosphere peaked in the second half of the 1990s. We examine the trends before and after that peak to see if any change in trend is discernible. The previously reported decreases are confirmed. Furthermore, the downward trend in upper stratospheric ozone has not continued. The possible significance of any increase is discussed in detail.
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.
M. J. Ashfold, J. A. Pyle, A. D. Robinson, E. Meneguz, M. S. M. Nadzir, S. M. Phang, A. A. Samah, S. Ong, H. E. Ung, L. K. Peng, S. E. Yong, and N. R. P. Harris
Atmos. Chem. Phys., 15, 3565–3573, https://doi.org/10.5194/acp-15-3565-2015, https://doi.org/10.5194/acp-15-3565-2015, 2015
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We use observations and model calculations to show that "cold surges" occurring during Northern Hemisphere winter can rapidly transport East Asian pollution to equatorial Southeast Asia. As well as affecting atmospheric composition near the surface, we argue that strong convection can subsequently lift the polluted air masses to the tropical upper troposphere. This suggests a potentially important connection between midlatitude pollution sources and the lower stratosphere.
F. Tummon, B. Hassler, N. R. P. Harris, J. Staehelin, W. Steinbrecht, J. Anderson, G. E. Bodeker, A. Bourassa, S. M. Davis, D. Degenstein, S. M. Frith, L. Froidevaux, E. Kyrölä, M. Laine, C. Long, A. A. Penckwitt, C. E. Sioris, K. H. Rosenlof, C. Roth, H.-J. Wang, and J. Wild
Atmos. Chem. Phys., 15, 3021–3043, https://doi.org/10.5194/acp-15-3021-2015, https://doi.org/10.5194/acp-15-3021-2015, 2015
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Understanding ozone trends in the vertical is vital in terms of assessing the success of the Montreal Protocol. This paper compares and analyses the long-term trends in stratospheric ozone from seven new merged satellite data sets. The data sets largely agree well with each other, particularly for the negative trends seen in the early period 1984-1997. For the 1998-2011 period there is less agreement, but a clear shift from negative to mostly positive trends.
P. Bergamaschi, M. Corazza, U. Karstens, M. Athanassiadou, R. L. Thompson, I. Pison, A. J. Manning, P. Bousquet, A. Segers, A. T. Vermeulen, G. Janssens-Maenhout, M. Schmidt, M. Ramonet, F. Meinhardt, T. Aalto, L. Haszpra, J. Moncrieff, M. E. Popa, D. Lowry, M. Steinbacher, A. Jordan, S. O'Doherty, S. Piacentino, and E. Dlugokencky
Atmos. Chem. Phys., 15, 715–736, https://doi.org/10.5194/acp-15-715-2015, https://doi.org/10.5194/acp-15-715-2015, 2015
S. J. O'Shea, G. Allen, M. W. Gallagher, K. Bower, S. M. Illingworth, J. B. A. Muller, B. T. Jones, C. J. Percival, S. J-B. Bauguitte, M. Cain, N. Warwick, A. Quiquet, U. Skiba, J. Drewer, K. Dinsmore, E. G. Nisbet, D. Lowry, R. E. Fisher, J. L. France, M. Aurela, A. Lohila, G. Hayman, C. George, D. B. Clark, A. J. Manning, A. D. Friend, and J. Pyle
Atmos. Chem. Phys., 14, 13159–13174, https://doi.org/10.5194/acp-14-13159-2014, https://doi.org/10.5194/acp-14-13159-2014, 2014
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This paper presents airborne measurements of greenhouse gases collected in the European Arctic. Regional scale flux estimates for the northern Scandinavian wetlands are derived. These fluxes are found to be in excellent agreement with coincident surface measurements within the aircraft's sampling domain. This has allowed a significant low bias to be identified in two commonly used process-based land surface models.
X. Yang, N. L. Abraham, A. T. Archibald, P. Braesicke, J. Keeble, P. J. Telford, N. J. Warwick, and J. A. Pyle
Atmos. Chem. Phys., 14, 10431–10438, https://doi.org/10.5194/acp-14-10431-2014, https://doi.org/10.5194/acp-14-10431-2014, 2014
S. O'Doherty, M. Rigby, J. Mühle, D. J. Ivy, B. R. Miller, D. Young, P. G. Simmonds, S. Reimann, M. K. Vollmer, P. B. Krummel, P. J. Fraser, L. P. Steele, B. Dunse, P. K. Salameh, C. M. Harth, T. Arnold, R. F. Weiss, J. Kim, S. Park, S. Li, C. Lunder, O. Hermansen, N. Schmidbauer, L. X. Zhou, B. Yao, R. H. J. Wang, A. J. Manning, and R. G. Prinn
Atmos. Chem. Phys., 14, 9249–9258, https://doi.org/10.5194/acp-14-9249-2014, https://doi.org/10.5194/acp-14-9249-2014, 2014
A. D. Robinson, N. R. P. Harris, M. J. Ashfold, B. Gostlow, N. J. Warwick, L. M. O'Brien, E. J. Beardmore, M. S. M. Nadzir, S. M. Phang, A. A. Samah, S. Ong, H. E. Ung, L. K. Peng, S. E. Yong, M. Mohamad, and J. A. Pyle
Atmos. Chem. Phys., 14, 8369–8388, https://doi.org/10.5194/acp-14-8369-2014, https://doi.org/10.5194/acp-14-8369-2014, 2014
M. S. Mohd Nadzir, S. M. Phang, M. R. Abas, N. Abdul Rahman, A. Abu Samah, W. T. Sturges, D. E. Oram, G. P. Mills, Emma C. Leedham Elvidge, J. A. Pyle, N. R. P. Harris, A. D. Robinson, M. J. Ashfold, M. I. Mead, M. T. Latif, M. F. Khan, A. M. Amiruddin, N. Banan, and M. M. Hanafiah
Atmos. Chem. Phys., 14, 8137–8148, https://doi.org/10.5194/acp-14-8137-2014, https://doi.org/10.5194/acp-14-8137-2014, 2014
Z. S. Stock, M. R. Russo, and J. A. Pyle
Atmos. Chem. Phys., 14, 3899–3912, https://doi.org/10.5194/acp-14-3899-2014, https://doi.org/10.5194/acp-14-3899-2014, 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
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
N. J. Warwick, A. T. Archibald, K. Ashworth, J. Dorsey, P. M. Edwards, D. E. Heard, B. Langford, J. Lee, P. K. Misztal, L. K. Whalley, and J. A. Pyle
Atmos. Chem. Phys., 13, 9183–9194, https://doi.org/10.5194/acp-13-9183-2013, https://doi.org/10.5194/acp-13-9183-2013, 2013
F. Ziska, B. Quack, K. Abrahamsson, S. D. Archer, E. Atlas, T. Bell, J. H. Butler, L. J. Carpenter, C. E. Jones, N. R. P. Harris, H. Hepach, K. G. Heumann, C. Hughes, J. Kuss, K. Krüger, P. Liss, R. M. Moore, A. Orlikowska, S. Raimund, C. E. Reeves, W. Reifenhäuser, A. D. Robinson, C. Schall, T. Tanhua, S. Tegtmeier, S. Turner, L. Wang, D. Wallace, J. Williams, H. Yamamoto, S. Yvon-Lewis, and Y. Yokouchi
Atmos. Chem. Phys., 13, 8915–8934, https://doi.org/10.5194/acp-13-8915-2013, https://doi.org/10.5194/acp-13-8915-2013, 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
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Physics (physical properties and processes)
On the uncertainty of anthropogenic aromatic volatile organic compound emissions: model evaluation and sensitivity analysis
A mechanism of stratospheric O3 intrusion into the atmospheric environment: a case study of the North China Plain
Influence of atmospheric circulation on the interannual variability of transport from global and regional emissions into the Arctic
Surface networks in the Arctic may miss a future methane bomb
Potential of using CO2 observations over India in a regional carbon budget estimation by improving the modelling system
A bottom-up emission estimate for the 2022 Nord Stream gas leak: derivation, simulations, and evaluation
European CH4 inversions with ICON-ART coupled to the CarbonTracker Data Assimilation Shell
Spatiotemporal Source Apportionment of Ozone Pollution over the Greater Bay Area
Extreme weather exacerbates ozone pollution in the Pearl River Delta, China: role of natural processes
Multidecadal ozone trends in China and implications for human health and crop yields: a hybrid approach combining a chemical transport model and machine learning
On the influence of vertical mixing, boundary layer schemes, and temporal emission profiles on tropospheric NO2 in WRF-Chem – comparisons to in situ, satellite, and MAX-DOAS observations
Decreasing trends of ammonia emissions over Europe seen from remote sensing and inverse modelling
The sensitivity of Southern Ocean atmospheric dimethyl sulfide (DMS) to modeled oceanic DMS concentrations and emissions
Impacts of maritime shipping on air pollution along the US East Coast
Understanding greenhouse gas (GHG) column concentrations in Munich using the Weather Research and Forecasting (WRF) model
Impact of transport model resolution and a priori assumptions on inverse modeling of Swiss F-gas emissions
Estimation of power plant SO2 emissions using the HYSPLIT dispersion model and airborne observations with plume rise ensemble runs
Can we use atmospheric CO2 measurements to verify emission trends reported by cities? Lessons from a 6-year atmospheric inversion over Paris
A new steady-state gas–particle partitioning model of polycyclic aromatic hydrocarbons: implication for the influence of the particulate proportion in emissions
An analysis of CMAQ gas-phase dry deposition over North America through grid-scale and land-use-specific diagnostics in the context of AQMEII4
Rethinking the role of transport and photochemistry in regional ozone pollution: insights from ozone concentration and mass budgets
Decreasing seasonal cycle amplitude of methane in the northern high latitudes being driven by lower-latitude changes in emissions and transport
Potential of 14C-based versus ∆CO-based ∆ffCO2 observations to estimate urban fossil fuel CO2 (ffCO2) emissions
The effect of anthropogenic emission, meteorological factors, and carbon dioxide on the surface ozone increase in China from 2008 to 2018 during the East Asia summer monsoon season
Development of a CMAQ–PMF-based composite index for prescribing an effective ozone abatement strategy: a case study of sensitivity of surface ozone to precursor volatile organic compound species in southern Taiwan
Comment on “Climate consequences of hydrogen emissions” by Ocko and Hamburg (2022)
Constraining emissions of volatile organic compounds from western US wildfires with WE-CAN and FIREX-AQ airborne observations
Satellite quantification of methane emissions and oil–gas methane intensities from individual countries in the Middle East and North Africa: implications for climate action
Coupled mesoscale–microscale modeling of air quality in a polluted city using WRF-LES-Chem
Impact of aerosol optics on vertical distribution of ozone in autumn over Yangtze River Delta
A view of the European carbon flux landscape through the lens of the ICOS atmospheric observation network
Technical note: The CAMS greenhouse gas reanalysis from 2003 to 2020
Evaluation of simulated CO2 power plant plumes from six high-resolution atmospheric transport models
Impacts of urbanization on air quality and the related health risks in a city with complex terrain
Optimizing 4 years of CO2 biospheric fluxes from OCO-2 and in situ data in TM5: fire emissions from GFED and inferred from MOPITT CO data
Development and application of a multi-scale modeling framework for urban high-resolution NO2 pollution mapping
Towards monitoring the CO2 source–sink distribution over India via inverse modelling: quantifying the fine-scale spatiotemporal variability in the atmospheric CO2 mole fraction
Methane emissions from China: a high-resolution inversion of TROPOMI satellite observations
Estimated regional CO2 flux and uncertainty based on an ensemble of atmospheric CO2 inversions
Assessing the representativity of NH3 measurements influenced by boundary-layer dynamics and the turbulent dispersion of a nearby emission source
Analysis of CO2, CH4, and CO surface and column concentrations observed at Réunion Island by assessing WRF-Chem simulations
Technical note: Interpretation of field observations of point-source methane plume using observation-driven large-eddy simulations
Quantifying fossil fuel methane emissions using observations of atmospheric ethane and an uncertain emission ratio
The impact of peripheral circulation characteristics of typhoon on sustained ozone episodes over the Pearl River Delta region, China
Updated Global Fuel Exploitation Inventory (GFEI) for methane emissions from the oil, gas, and coal sectors: evaluation with inversions of atmospheric methane observations
High-resolution mapping of regional traffic emissions using land-use machine learning models
Land use and anthropogenic heat modulate ozone by meteorology: a perspective from the Yangtze River Delta region
Four years of global carbon cycle observed from the Orbiting Carbon Observatory 2 (OCO-2) version 9 and in situ data and comparison to OCO-2 version 7
Data assimilation of CrIS NH3 satellite observations for improving spatiotemporal NH3 distributions in LOTOS-EUROS
On the cross-tropopause transport of water by tropical convective overshoots: a mesoscale modelling study constrained by in situ observations during the TRO-Pico field campaign in Brazil
Kevin Oliveira, Marc Guevara, Oriol Jorba, Hervé Petetin, Dene Bowdalo, Carles Tena, Gilbert Montané Pinto, Franco López, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 7137–7177, https://doi.org/10.5194/acp-24-7137-2024, https://doi.org/10.5194/acp-24-7137-2024, 2024
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In this work, we assess and evaluate benzene, toluene, and xylene primary emissions and air quality levels in Spain by combining observations, emission inventories, and air quality modelling techniques. The comparison between modelled and observed levels allows identifying uncertainty sources within the emission input. This contributes to improving air quality models' performance when simulating these compounds, leading to better support for the design of effective pollution control strategies.
Yuehan Luo, Tianliang Zhao, Kai Meng, Jun Hu, Qingjian Yang, Yongqing Bai, Kai Yang, Weikang Fu, Chenghao Tan, Yifan Zhang, Yanzhe Zhang, and Zhikuan Li
Atmos. Chem. Phys., 24, 7013–7026, https://doi.org/10.5194/acp-24-7013-2024, https://doi.org/10.5194/acp-24-7013-2024, 2024
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We reveal a significant mechanism of stratospheric O3 intrusion (SI) into the atmospheric environment induced by an extratropical cyclone system. This system facilitates the downward transport of stratospheric O3 to the near-surface layer by vertical coupling, involving the upper westerly trough, the middle northeast cold vortex, and the lower extratropical cyclone in the troposphere. On average, stratospheric O3 contributed 26.77 % to near-surface O3 levels over the North China Plain.
Cheng Zheng, Yutian Wu, Mingfang Ting, and Clara Orbe
Atmos. Chem. Phys., 24, 6965–6985, https://doi.org/10.5194/acp-24-6965-2024, https://doi.org/10.5194/acp-24-6965-2024, 2024
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Trace gases and aerosols in the Arctic, which typically originate from midlatitude and tropical emission regions, modulate the Arctic climate via their radiative and chemistry impacts. Thus, long-range transport of these substances is important for understanding the current and the future change of Arctic climate. By employing chemistry–climate models, we explore how year-to-year variations in the atmospheric circulation modulate atmospheric long-range transport into the Arctic.
Sophie Wittig, Antoine Berchet, Isabelle Pison, Marielle Saunois, and Jean-Daniel Paris
Atmos. Chem. Phys., 24, 6359–6373, https://doi.org/10.5194/acp-24-6359-2024, https://doi.org/10.5194/acp-24-6359-2024, 2024
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The aim of this work is to analyse how accurately a methane bomb event could be detected with the current and a hypothetically extended stationary observation network in the Arctic. For this, we incorporate synthetically modelled possible future CH4 concentrations based on plausible emission scenarios into an inverse modelling framework. We analyse how well the increase is detected in different Arctic regions and evaluate the impact of additional observation sites in this respect.
Vishnu Thilakan, Dhanyalekshmi Pillai, Jithin Sukumaran, Christoph Gerbig, Haseeb Hakkim, Vinayak Sinha, Yukio Terao, Manish Naja, and Monish Vijay Deshpande
Atmos. Chem. Phys., 24, 5315–5335, https://doi.org/10.5194/acp-24-5315-2024, https://doi.org/10.5194/acp-24-5315-2024, 2024
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This study investigates the usability of CO2 mixing ratio observations over India to infer regional carbon sources and sinks. We demonstrate that a high-resolution modelling system can represent the observed CO2 variations reasonably well by improving the transport and flux variations at a fine scale. Future carbon data assimilation systems can thus benefit from these recently available CO2 observations when fine-scale variations are adequately represented in the models.
Rostislav Kouznetsov, Risto Hänninen, Andreas Uppstu, Evgeny Kadantsev, Yalda Fatahi, Marje Prank, Dmitrii Kouznetsov, Steffen Manfred Noe, Heikki Junninen, and Mikhail Sofiev
Atmos. Chem. Phys., 24, 4675–4691, https://doi.org/10.5194/acp-24-4675-2024, https://doi.org/10.5194/acp-24-4675-2024, 2024
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By relying solely on publicly available media reports, we were able to infer the temporal evolution and the injection height for the Nord Stream gas leaks in September 2022. The inventory specifies locations, vertical distributions, and temporal evolution of the methane sources. The inventory can be used to simulate the event with atmospheric transport models. The inventory is supplemented with a set of observational data tailored to evaluate the results of the simulated atmospheric dispersion.
Michael Steiner, Wouter Peters, Ingrid Luijkx, Stephan Henne, Huilin Chen, Samuel Hammer, and Dominik Brunner
Atmos. Chem. Phys., 24, 2759–2782, https://doi.org/10.5194/acp-24-2759-2024, https://doi.org/10.5194/acp-24-2759-2024, 2024
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The Paris Agreement increased interest in estimating greenhouse gas (GHG) emissions of individual countries, but top-down emission estimation is not yet considered policy-relevant. It is therefore paramount to reduce large errors and to build systems that are based on the newest atmospheric transport models. In this study, we present the first application of ICON-ART in the inverse modeling of GHG fluxes with an ensemble Kalman filter and present our results for European CH4 emissions.
Yiang Chen, Xingcheng Lu, and Jimmy C. H. Fung
EGUsphere, https://doi.org/10.5194/egusphere-2023-3140, https://doi.org/10.5194/egusphere-2023-3140, 2024
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This study investigates the contribution of pollutants from different emitting periods to ozone episodes over the Greater Bay Area. The analysis reveals the variation of major spatiotemporal contributors to the O3 pollution under the influence of typhoons and sub-tropical high-pressure. Through the temporal contribution analysis, our work offers a new perspective on the evolution of O3 pollution and can aid in developing effective and timely control policies under unfavorable weather conditions.
Nan Wang, Hongyue Wang, Xin Huang, Xi Chen, Yu Zou, Tao Deng, Tingyuan Li, Xiaopu Lyu, and Fumo Yang
Atmos. Chem. Phys., 24, 1559–1570, https://doi.org/10.5194/acp-24-1559-2024, https://doi.org/10.5194/acp-24-1559-2024, 2024
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This study explores the influence of extreme-weather-induced natural processes on ozone pollution, which is often overlooked. By analyzing meteorological factors, natural emissions, chemistry pathways and atmospheric transport, we discovered that these natural processes could substantially exacerbate ozone pollution. The findings contribute to a deeper understanding of ozone pollution and offer valuable insights for controlling ozone pollution in the context of global warming.
Jia Mao, Amos P. K. Tai, David H. Y. Yung, Tiangang Yuan, Kong T. Chau, and Zhaozhong Feng
Atmos. Chem. Phys., 24, 345–366, https://doi.org/10.5194/acp-24-345-2024, https://doi.org/10.5194/acp-24-345-2024, 2024
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Surface ozone (O3) is well-known for posing great threats to both human health and agriculture worldwide. However, a multidecadal assessment of the impacts of O3 on public health and agriculture in China is lacking without sufficient O3 observations. We used a hybrid approach combining a chemical transport model and machine learning to provide a robust dataset of O3 concentrations over the past 4 decades in China, thereby filling the gap in the long-term O3 trend and impact assessment in China.
Leon Kuhn, Steffen Beirle, Vinod Kumar, Sergey Osipov, Andrea Pozzer, Tim Bösch, Rajesh Kumar, and Thomas Wagner
Atmos. Chem. Phys., 24, 185–217, https://doi.org/10.5194/acp-24-185-2024, https://doi.org/10.5194/acp-24-185-2024, 2024
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NO₂ is an important air pollutant. It was observed that the WRF-Chem model shows significant deviations in NO₂ abundance when compared to measurements. We use a 1-month simulation over central Europe to show that these deviations can be mostly resolved by reparameterization of the vertical mixing routine. In order to validate our results, they are compared to in situ, satellite, and MAX-DOAS measurements.
Ondřej Tichý, Sabine Eckhardt, Yves Balkanski, Didier Hauglustaine, and Nikolaos Evangeliou
Atmos. Chem. Phys., 23, 15235–15252, https://doi.org/10.5194/acp-23-15235-2023, https://doi.org/10.5194/acp-23-15235-2023, 2023
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We show declining trends in NH3 emissions over Europe for 2013–2020 using advanced dispersion and inverse modelling and satellite measurements from CrIS. Emissions decreased by −26% since 2013, showing that the abatement strategies adopted by the European Union have been very efficient. Ammonia emissions are low in winter and peak in summer due to temperature-dependent soil volatilization. The largest decreases were observed in central and western Europe in countries with high emissions.
Yusuf A. Bhatti, Laura E. Revell, Alex J. Schuddeboom, Adrian J. McDonald, Alex T. Archibald, Jonny Williams, Abhijith U. Venugopal, Catherine Hardacre, and Erik Behrens
Atmos. Chem. Phys., 23, 15181–15196, https://doi.org/10.5194/acp-23-15181-2023, https://doi.org/10.5194/acp-23-15181-2023, 2023
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Aerosols are a large source of uncertainty over the Southern Ocean. A dominant source of sulfate aerosol in this region is dimethyl sulfide (DMS), which is poorly simulated by climate models. We show the sensitivity of simulated atmospheric DMS to the choice of oceanic DMS data set and emission scheme. We show that oceanic DMS has twice the influence on atmospheric DMS than the emission scheme. Simulating DMS more accurately in climate models will help to constrain aerosol uncertainty.
Maryam Golbazi and Cristina Archer
Atmos. Chem. Phys., 23, 15057–15075, https://doi.org/10.5194/acp-23-15057-2023, https://doi.org/10.5194/acp-23-15057-2023, 2023
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We use scientific models to study the impact of ship emissions on air quality along the US East Coast. We find an increase in three major pollutants (PM2.5, NO2, and SO2) in coastal regions. However, we detect a reduction in ozone (O3) levels in major coastal cities. This reduction is linked to the significant emissions of nitrogen oxides (NOx) from ships, which scavenged O3, especially in highly polluted urban areas experiencing an NOx-limited regime.
Xinxu Zhao, Jia Chen, Julia Marshall, Michal Gałkowski, Stephan Hachinger, Florian Dietrich, Ankit Shekhar, Johannes Gensheimer, Adrian Wenzel, and Christoph Gerbig
Atmos. Chem. Phys., 23, 14325–14347, https://doi.org/10.5194/acp-23-14325-2023, https://doi.org/10.5194/acp-23-14325-2023, 2023
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We develop a modeling framework using the Weather Research and Forecasting model at a high spatial resolution (up to 400 m) to simulate atmospheric transport of greenhouse gases and interpret column observations. Output is validated against weather stations and column measurements in August 2018. The differential column method is applied, aided by air-mass transport tracing with the Stochastic Time-Inverted Lagrangian Transport (STILT) model, also for an exploratory measurement interpretation.
Ioannis Katharopoulos, Dominique Rust, Martin K. Vollmer, Dominik Brunner, Stefan Reimann, Simon J. O'Doherty, Dickon Young, Kieran M. Stanley, Tanja Schuck, Jgor Arduini, Lukas Emmenegger, and Stephan Henne
Atmos. Chem. Phys., 23, 14159–14186, https://doi.org/10.5194/acp-23-14159-2023, https://doi.org/10.5194/acp-23-14159-2023, 2023
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The effectiveness of climate change mitigation needs to be scrutinized by monitoring greenhouse gas (GHG) emissions. Countries report their emissions to the UN in a bottom-up manner. By combining atmospheric observations and transport models someone can independently validate emission estimates in a top-down fashion. We report Swiss emissions of synthetic GHGs based on kilometer-scale transport and inverse modeling, highlighting the role of appropriate resolution in complex terrain.
Tianfeng Chai, Xinrong Ren, Fong Ngan, Mark Cohen, and Alice Crawford
Atmos. Chem. Phys., 23, 12907–12933, https://doi.org/10.5194/acp-23-12907-2023, https://doi.org/10.5194/acp-23-12907-2023, 2023
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The SO2 emissions of three power plants are estimated using aircraft observations and an ensemble of HYSPLIT dispersion simulations with different plume rise parameters. The emission estimates using the runs with the lowest root mean square errors (RMSEs) and the runs with the best correlation coefficients between the predicted and observed mixing ratios both agree well with the Continuous Emissions Monitoring Systems (CEMS) data. The RMSE-based plume rise appears to be more reasonable.
Jinghui Lian, Thomas Lauvaux, Hervé Utard, François-Marie Bréon, Grégoire Broquet, Michel Ramonet, Olivier Laurent, Ivonne Albarus, Mali Chariot, Simone Kotthaus, Martial Haeffelin, Olivier Sanchez, Olivier Perrussel, Hugo Anne Denier van der Gon, Stijn Nicolaas Camiel Dellaert, and Philippe Ciais
Atmos. Chem. Phys., 23, 8823–8835, https://doi.org/10.5194/acp-23-8823-2023, https://doi.org/10.5194/acp-23-8823-2023, 2023
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This study quantifies urban CO2 emissions via an atmospheric inversion for the Paris metropolitan area over a 6-year period from 2016 to 2021. Results show a long-term decreasing trend of about 2 % ± 0.6 % per year in the annual CO2 emissions over Paris. We conclude that our current capacity can deliver near-real-time CO2 emission estimates at the city scale in under a month, and the results agree within 10 % with independent estimates from multiple city-scale inventories.
Fu-Jie Zhu, Peng-Tuan Hu, and Wan-Li Ma
Atmos. Chem. Phys., 23, 8583–8590, https://doi.org/10.5194/acp-23-8583-2023, https://doi.org/10.5194/acp-23-8583-2023, 2023
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A new steady-state gas–particle partitioning model of polycyclic aromatic hydrocarbons was established based on the level-III multimedia fugacity model, which proved that the particulate proportion of PAHs in emissions was a crucial factor for G–P partitioning of PAHs. In addition, gaseous and particulate interference was also derived in the new steady-state model determined by the particulate proportion in emission that could derivate the G–P partitioning quotients from the equilibrium state.
Christian Hogrefe, Jesse O. Bash, Jonathan E. Pleim, Donna B. Schwede, Robert C. Gilliam, Kristen M. Foley, K. Wyat Appel, and Rohit Mathur
Atmos. Chem. Phys., 23, 8119–8147, https://doi.org/10.5194/acp-23-8119-2023, https://doi.org/10.5194/acp-23-8119-2023, 2023
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Under the umbrella of the fourth phase of the Air Quality Model Evaluation International Initiative (AQMEII4), this study applies AQMEII4 diagnostic tools to better characterize how dry deposition removes pollutants from the atmosphere in the widely used CMAQ model. The results illustrate how these tools can provide insights into similarities and differences between the two CMAQ dry deposition options that affect simulated pollutant budgets and ecosystem impacts from atmospheric pollution.
Kun Qu, Xuesong Wang, Xuhui Cai, Yu Yan, Xipeng Jin, Mihalis Vrekoussis, Maria Kanakidou, Guy P. Brasseur, Jin Shen, Teng Xiao, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 23, 7653–7671, https://doi.org/10.5194/acp-23-7653-2023, https://doi.org/10.5194/acp-23-7653-2023, 2023
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Basic understandings of ozone processes, especially transport and chemistry, are essential to support ozone pollution control, but studies often have different views on their relative importance. We developed a method to quantify their contributions in the ozone mass and concentration budgets based on the WRF-CMAQ model. Results in a polluted region highlight the differences between two budgets. For future studies, two budgets are both needed to fully understand the effects of ozone processes.
Emily Dowd, Chris Wilson, Martyn P. Chipperfield, Emanuel Gloor, Alistair Manning, and Ruth Doherty
Atmos. Chem. Phys., 23, 7363–7382, https://doi.org/10.5194/acp-23-7363-2023, https://doi.org/10.5194/acp-23-7363-2023, 2023
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Surface observations of methane show that the seasonal cycle amplitude (SCA) of methane is decreasing in the northern high latitudes (NHLs) but increased globally (1995–2020). The NHL decrease is counterintuitive, as we expect the SCA to increase with increasing concentrations. We use a chemical transport model to investigate changes in SCA in the NHLs. We find well-mixed methane and changes in emissions from Canada, the Middle East, and Europe are the largest contributors to the SCA in NHLs.
Fabian Manuel Maier, Christian Rödenbeck, Ingeborg Levin, Christoph Gerbig, Maksym Gachkivskyi, and Samuel Hammer
EGUsphere, https://doi.org/10.5194/egusphere-2023-1239, https://doi.org/10.5194/egusphere-2023-1239, 2023
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We investigate the usage of discrete radiocarbon (14C)-based fossil fuel carbon dioxide (ffCO2) concentration estimates versus continuous carbon monoxide (CO)-based ffCO2 estimates to evaluate the seasonal cycle of the ffCO2 emissions in an urban region with an inverse modelling framework. We find that the CO-based ffCO2 estimates allow to reconstruct robust seasonal cycles, which show the distinct Covid-19 drawdown in 2020 and can be used to validate emission inventories.
Danyang Ma, Tijian Wang, Hao Wu, Yawei Qu, Jian Liu, Jane Liu, Shu Li, Bingliang Zhuang, Mengmeng Li, and Min Xie
Atmos. Chem. Phys., 23, 6525–6544, https://doi.org/10.5194/acp-23-6525-2023, https://doi.org/10.5194/acp-23-6525-2023, 2023
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Increasing surface ozone (O3) concentrations have long been a significant environmental issue in China, despite the Clean Air Action Plan launched in 2013. Most previous research ignores the contributions of CO2 variations. Our study comprehensively analyzed O3 variation across China from various perspectives and highlighted the importance of considering CO2 variations when designing long-term O3 control policies, especially in high-vegetation-coverage areas.
Jackson Hian-Wui Chang, Stephen M. Griffith, Steven Soon-Kai Kong, Ming-Tung Chuang, and Neng-Huei Lin
Atmos. Chem. Phys., 23, 6357–6382, https://doi.org/10.5194/acp-23-6357-2023, https://doi.org/10.5194/acp-23-6357-2023, 2023
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A novel CMAQ–PMF-based composite index is developed to identify the key VOC source species for an effective ozone abatement strategy. The index provides information as to which VOC species are key to ozone formation and where to reduce sources of these VOC species. Using the composite index, we recommended the VOC control measures in southern Taiwan should prioritize solvent usage, vehicle emissions, and the petrochemical industry.
Lei Duan and Ken Caldeira
Atmos. Chem. Phys., 23, 6011–6020, https://doi.org/10.5194/acp-23-6011-2023, https://doi.org/10.5194/acp-23-6011-2023, 2023
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Ocko and Hamburg (2022) emphasize the short-term climate impact of hydrogen, and we present an analysis that places greater focus on long-term outcomes. We have derived equations that describe the time-evolving impact of hydrogen and show that higher methane leakage is primarily responsible for the warming potential of blue hydrogen, while hydrogen leakage plays a less critical role. Fossil fuels show more prominent longer-term climate impacts than clean hydrogen under all emission scenarios.
Lixu Jin, Wade Permar, Vanessa Selimovic, Damien Ketcherside, Robert J. Yokelson, Rebecca S. Hornbrook, Eric C. Apel, I-Ting Ku, Jeffrey L. Collett Jr., Amy P. Sullivan, Daniel A. Jaffe, Jeffrey R. Pierce, Alan Fried, Matthew M. Coggon, Georgios I. Gkatzelis, Carsten Warneke, Emily V. Fischer, and Lu Hu
Atmos. Chem. Phys., 23, 5969–5991, https://doi.org/10.5194/acp-23-5969-2023, https://doi.org/10.5194/acp-23-5969-2023, 2023
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Air quality in the USA has been improving since 1970 due to anthropogenic emission reduction. Those gains have been partly offset by increased wildfire pollution in the western USA in the past 20 years. Still, we do not understand wildfire emissions well due to limited measurements. Here, we used a global transport model to evaluate and constrain current knowledge of wildfire emissions with recent observational constraints, showing the underestimation of wildfire emissions in the western USA.
Zichong Chen, Daniel J. Jacob, Ritesh Gautam, Mark Omara, Robert N. Stavins, Robert C. Stowe, Hannah Nesser, Melissa P. Sulprizio, Alba Lorente, Daniel J. Varon, Xiao Lu, Lu Shen, Zhen Qu, Drew C. Pendergrass, and Sarah Hancock
Atmos. Chem. Phys., 23, 5945–5967, https://doi.org/10.5194/acp-23-5945-2023, https://doi.org/10.5194/acp-23-5945-2023, 2023
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We quantify methane emissions from individual countries in the Middle East and North Africa by inverse analysis of 2019 TROPOMI satellite observations of atmospheric methane. We show that the ability to simply relate oil/gas emissions to activity metrics is compromised by stochastic nature of local infrastructure and management practices. We find that the industry target for oil/gas methane intensity is achievable through associated gas capture, modern infrastructure, and centralized operations.
Yuting Wang, Yong-Feng Ma, Domingo Muñoz-Esparza, Jianing Dai, Cathy Wing Yi Li, Pablo Lichtig, Roy Chun-Wang Tsang, Chun-Ho Liu, Tao Wang, and Guy Pierre Brasseur
Atmos. Chem. Phys., 23, 5905–5927, https://doi.org/10.5194/acp-23-5905-2023, https://doi.org/10.5194/acp-23-5905-2023, 2023
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Air quality in urban areas is difficult to simulate in coarse-resolution models. This work exploits the WRF (Weather Research and Forecasting) model coupled with a large-eddy simulation (LES) component and online chemistry to perform high-resolution (33.3 m) simulations of air quality in a large city. The evaluation of the simulations with observations shows that increased model resolution improves the representation of the chemical species near the pollution sources.
Shuqi Yan, Bin Zhu, Shuangshuang Shi, Wen Lu, Jinhui Gao, Hanqing Kang, and Duanyang Liu
Atmos. Chem. Phys., 23, 5177–5190, https://doi.org/10.5194/acp-23-5177-2023, https://doi.org/10.5194/acp-23-5177-2023, 2023
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We analyze ozone response to aerosol mixing states in the vertical direction by WRF-Chem simulations. Aerosols generally lead to turbulent suppression, precursor accumulation, low-level photolysis reduction, and upper-level photolysis enhancement under different underlying surface and pollution conditions. Thus, ozone decreases within the entire boundary layer during the daytime, and the decrease is the least in aerosol external mixing states compared to internal and core shell mixing states.
Ida Storm, Ute Karstens, Claudio D'Onofrio, Alex Vermeulen, and Wouter Peters
Atmos. Chem. Phys., 23, 4993–5008, https://doi.org/10.5194/acp-23-4993-2023, https://doi.org/10.5194/acp-23-4993-2023, 2023
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In this study, we evaluate what is in the influence regions of the ICOS atmospheric measurement stations to gain insight into what land cover types and land-cover-associated fluxes the network represents. Subsequently, insights about strengths, weaknesses, and potential gaps can assist in future network expansion decisions. The network is concentrated in central Europe, which leads to a general overrepresentation of coniferous forest and cropland and underrepresentation of grass and shrubland.
Anna Agustí-Panareda, Jérôme Barré, Sébastien Massart, Antje Inness, Ilse Aben, Melanie Ades, Bianca C. Baier, Gianpaolo Balsamo, Tobias Borsdorff, Nicolas Bousserez, Souhail Boussetta, Michael Buchwitz, Luca Cantarello, Cyril Crevoisier, Richard Engelen, Henk Eskes, Johannes Flemming, Sébastien Garrigues, Otto Hasekamp, Vincent Huijnen, Luke Jones, Zak Kipling, Bavo Langerock, Joe McNorton, Nicolas Meilhac, Stefan Noël, Mark Parrington, Vincent-Henri Peuch, Michel Ramonet, Miha Razinger, Maximilian Reuter, Roberto Ribas, Martin Suttie, Colm Sweeney, Jérôme Tarniewicz, and Lianghai Wu
Atmos. Chem. Phys., 23, 3829–3859, https://doi.org/10.5194/acp-23-3829-2023, https://doi.org/10.5194/acp-23-3829-2023, 2023
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We present a global dataset of atmospheric CO2 and CH4, the two most important human-made greenhouse gases, which covers almost 2 decades (2003–2020). It is produced by combining satellite data of CO2 and CH4 with a weather and air composition prediction model, and it has been carefully evaluated against independent observations to ensure validity and point out deficiencies to the user. This dataset can be used for scientific studies in the field of climate change and the global carbon cycle.
Dominik Brunner, Gerrit Kuhlmann, Stephan Henne, Erik Koene, Bastian Kern, Sebastian Wolff, Christiane Voigt, Patrick Jöckel, Christoph Kiemle, Anke Roiger, Alina Fiehn, Sven Krautwurst, Konstantin Gerilowski, Heinrich Bovensmann, Jakob Borchardt, Michal Galkowski, Christoph Gerbig, Julia Marshall, Andrzej Klonecki, Pascal Prunet, Robert Hanfland, Margit Pattantyús-Ábrahám, Andrzej Wyszogrodzki, and Andreas Fix
Atmos. Chem. Phys., 23, 2699–2728, https://doi.org/10.5194/acp-23-2699-2023, https://doi.org/10.5194/acp-23-2699-2023, 2023
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We evaluated six atmospheric transport models for their capability to simulate the CO2 plumes from two of the largest power plants in Europe by comparing the models against aircraft observations collected during the CoMet (Carbon Dioxide and Methane Mission) campaign in 2018. The study analyzed how realistically such plumes can be simulated at different model resolutions and how well the planned European satellite mission CO2M will be able to quantify emissions from power plants.
Chenchao Zhan, Min Xie, Hua Lu, Bojun Liu, Zheng Wu, Tijian Wang, Bingliang Zhuang, Mengmeng Li, and Shu Li
Atmos. Chem. Phys., 23, 771–788, https://doi.org/10.5194/acp-23-771-2023, https://doi.org/10.5194/acp-23-771-2023, 2023
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With the development of urbanization, urban land use and anthropogenic
emissions increase, affecting urban air quality and, in turn, the health risks associated with air pollutants. In this study, we systematically evaluate the impacts of urbanization on air quality and the corresponding health risks in a highly urbanized city with severe air pollution and complex terrain. This work focuses on the health risks caused by urbanization and can provide valuable insight for air pollution strategies.
Hélène Peiro, Sean Crowell, and Berrien Moore III
Atmos. Chem. Phys., 22, 15817–15849, https://doi.org/10.5194/acp-22-15817-2022, https://doi.org/10.5194/acp-22-15817-2022, 2022
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CO data can provide a powerful constraint on fire fluxes, supporting more accurate estimation of biospheric CO2 fluxes. We converted CO fire flux into CO2 fire prior, which is then used to adjust CO2 respiration. We applied this to two other fire flux products. CO2 inversions constrained by satellites or in situ data are then performed. Results show larger variations among the data assimilated than across the priors, but tropical flux from in situ inversions is sensitive to priors.
Zhaofeng Lv, Zhenyu Luo, Fanyuan Deng, Xiaotong Wang, Junchao Zhao, Lucheng Xu, Tingkun He, Yingzhi Zhang, Huan Liu, and Kebin He
Atmos. Chem. Phys., 22, 15685–15702, https://doi.org/10.5194/acp-22-15685-2022, https://doi.org/10.5194/acp-22-15685-2022, 2022
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This study developed a hybrid model, CMAQ-RLINE_URBAN, to predict the urban NO2 concentrations at a high spatial resolution. To estimate the influence of various street canyons on the dispersion of air pollutants, a new parameterization scheme was established based on computational fluid dynamics and machine learning methods. This work created a new method to identify the characteristics of vehicle-related air pollution at both city and street scales simultaneously and accurately.
Vishnu Thilakan, Dhanyalekshmi Pillai, Christoph Gerbig, Michal Galkowski, Aparnna Ravi, and Thara Anna Mathew
Atmos. Chem. Phys., 22, 15287–15312, https://doi.org/10.5194/acp-22-15287-2022, https://doi.org/10.5194/acp-22-15287-2022, 2022
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This paper demonstrates how we can use atmospheric observations to improve the CO2 flux estimates in India. This is achieved by improving the representation of terrain, mesoscale transport, and flux variations. We quantify the impact of the unresolved variations in the current models on optimally estimated fluxes via inverse modelling and quantify the associated flux uncertainty. We illustrate how a parameterization scheme captures this variability in the coarse models.
Zichong Chen, Daniel J. Jacob, Hannah Nesser, Melissa P. Sulprizio, Alba Lorente, Daniel J. Varon, Xiao Lu, Lu Shen, Zhen Qu, Elise Penn, and Xueying Yu
Atmos. Chem. Phys., 22, 10809–10826, https://doi.org/10.5194/acp-22-10809-2022, https://doi.org/10.5194/acp-22-10809-2022, 2022
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We quantify methane emissions in China and contributions from different sectors by inverse analysis of 2019 TROPOMI satellite observations of atmospheric methane. We find that anthropogenic methane emissions for China are underestimated in the national inventory. Our estimate of emissions indicates a small life-cycle loss rate, implying net climate benefits from the current
coal-to-gasenergy transition in China. However, this small loss rate can be misleading given China's high gas imports.
Naveen Chandra, Prabir K. Patra, Yousuke Niwa, Akihiko Ito, Yosuke Iida, Daisuke Goto, Shinji Morimoto, Masayuki Kondo, Masayuki Takigawa, Tomohiro Hajima, and Michio Watanabe
Atmos. Chem. Phys., 22, 9215–9243, https://doi.org/10.5194/acp-22-9215-2022, https://doi.org/10.5194/acp-22-9215-2022, 2022
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This paper is intended to accomplish two goals: (1) quantify mean and uncertainty in non-fossil-fuel CO2 fluxes estimated by inverse modeling and (2) provide in-depth analyses of regional CO2 fluxes in support of emission mitigation policymaking. CO2 flux variability and trends are discussed concerning natural climate variability and human disturbances using multiple lines of evidence.
Ruben B. Schulte, Margreet C. van Zanten, Bart J. H. van Stratum, and Jordi Vilà-Guerau de Arellano
Atmos. Chem. Phys., 22, 8241–8257, https://doi.org/10.5194/acp-22-8241-2022, https://doi.org/10.5194/acp-22-8241-2022, 2022
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We present a fine-scale simulation framework, utilizing large-eddy simulations, to assess NH3 measurements influenced by boundary-layer dynamics and turbulent dispersion of a nearby emission source. The minimum required distance from an emission source differs for concentration and flux measurements, from 0.5–3.0 km and 0.75–4.5 km, respectively. The simulation framework presented here proves to be a powerful and versatile tool for future NH3 research at high spatio-temporal resolutions.
Sieglinde Callewaert, Jérôme Brioude, Bavo Langerock, Valentin Duflot, Dominique Fonteyn, Jean-François Müller, Jean-Marc Metzger, Christian Hermans, Nicolas Kumps, Michel Ramonet, Morgan Lopez, Emmanuel Mahieu, and Martine De Mazière
Atmos. Chem. Phys., 22, 7763–7792, https://doi.org/10.5194/acp-22-7763-2022, https://doi.org/10.5194/acp-22-7763-2022, 2022
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A regional atmospheric transport model is used to analyze the factors contributing to CO2, CH4, and CO observations at Réunion Island. We show that the surface observations are dominated by local fluxes and dynamical processes, while the column data are influenced by larger-scale mechanisms such as biomass burning plumes. The model is able to capture the measured time series well; however, the results are highly dependent on accurate boundary conditions and high-resolution emission inventories.
Anja Ražnjević, Chiel van Heerwaarden, Bart van Stratum, Arjan Hensen, Ilona Velzeboer, Pim van den Bulk, and Maarten Krol
Atmos. Chem. Phys., 22, 6489–6505, https://doi.org/10.5194/acp-22-6489-2022, https://doi.org/10.5194/acp-22-6489-2022, 2022
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Mobile measurement techniques (e.g., instruments placed in cars) are often employed to identify and quantify individual sources of greenhouse gases. Due to road restrictions, those observations are often sparse (temporally and spatially). We performed high-resolution simulations of plume dispersion, with realistic weather conditions encountered in the field, to reproduce the measurement process of a methane plume emitted from an oil well and provide additional information about the plume.
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.
Ying Li, Xiangjun Zhao, Xuejiao Deng, and Jinhui Gao
Atmos. Chem. Phys., 22, 3861–3873, https://doi.org/10.5194/acp-22-3861-2022, https://doi.org/10.5194/acp-22-3861-2022, 2022
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This study finds a new phenomenon of weak wind deepening (WWD) associated with the peripheral circulation of typhoon and gives the influence mechanism of WWD on its contribution to daily variation during sustained ozone episodes. The WWD provides the premise for pollution accumulation in the whole PBL and continued enhancement of ground-level ozone via vertical mixing processes. These findings could benefit the daily daytime ozone forecast in the PRD region and other areas.
Tia R. Scarpelli, Daniel J. Jacob, Shayna Grossman, Xiao Lu, Zhen Qu, Melissa P. Sulprizio, Yuzhong Zhang, Frances Reuland, Deborah Gordon, and John R. Worden
Atmos. Chem. Phys., 22, 3235–3249, https://doi.org/10.5194/acp-22-3235-2022, https://doi.org/10.5194/acp-22-3235-2022, 2022
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We present a spatially explicit version of the national inventories of oil, gas, and coal methane emissions as submitted by individual countries to the United Nations Framework Convention on Climate Change (UNFCCC) in 2021. We then use atmospheric modeling to compare our inventory emissions to atmospheric methane observations with the goal of identifying potential under- and overestimates of oil–gas methane emissions in the national inventories.
Xiaomeng Wu, Daoyuan Yang, Ruoxi Wu, Jiajun Gu, Yifan Wen, Shaojun Zhang, Rui Wu, Renjie Wang, Honglei Xu, K. Max Zhang, Ye Wu, and Jiming Hao
Atmos. Chem. Phys., 22, 1939–1950, https://doi.org/10.5194/acp-22-1939-2022, https://doi.org/10.5194/acp-22-1939-2022, 2022
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Our work pioneered land-use machine learning methods for developing link-level emission inventories, utilizing hourly traffic profiles, including volume, speed, and fleet mix, obtained from the governmental intercity highway monitoring network in the "capital circles" of China. This research provides a platform to realize the near-real-time process of establishing high-resolution vehicle emission inventories for policy makers to engage in sophisticated traffic management.
Chenchao Zhan and Min Xie
Atmos. Chem. Phys., 22, 1351–1371, https://doi.org/10.5194/acp-22-1351-2022, https://doi.org/10.5194/acp-22-1351-2022, 2022
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The changes of land use and anthropogenic heat (AH) derived from urbanization can affect meteorology and in turn O3 evolution. In this study, we briefly describe the general features of O3 pollution in the Yangtze River Delta (YRD) based on in situ observational data. Then, the impacts of land use and anthropogenic heat on O3 via changing the meteorological factors and local circulations are investigated in this region using the WRF-Chem model.
Hélène Peiro, Sean Crowell, Andrew Schuh, David F. Baker, Chris O'Dell, Andrew R. Jacobson, Frédéric Chevallier, Junjie Liu, Annmarie Eldering, David Crisp, Feng Deng, Brad Weir, Sourish Basu, Matthew S. Johnson, Sajeev Philip, and Ian Baker
Atmos. Chem. Phys., 22, 1097–1130, https://doi.org/10.5194/acp-22-1097-2022, https://doi.org/10.5194/acp-22-1097-2022, 2022
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Satellite CO2 observations are constantly improved. We study an ensemble of different atmospheric models (inversions) from 2015 to 2018 using separate ground-based data or two versions of the OCO-2 satellite. Our study aims to determine if different satellite data corrections can yield different estimates of carbon cycle flux. A difference in the carbon budget between the two versions is found over tropical Africa, which seems to show the impact of corrections applied in satellite data.
Shelley van der Graaf, Enrico Dammers, Arjo Segers, Richard Kranenburg, Martijn Schaap, Mark W. Shephard, and Jan Willem Erisman
Atmos. Chem. Phys., 22, 951–972, https://doi.org/10.5194/acp-22-951-2022, https://doi.org/10.5194/acp-22-951-2022, 2022
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CrIS NH3 satellite observations are assimilated into the LOTOS-EUROS model using two different methods. In the first method the data are used to fit spatially varying NH3 emission time factors. In the second method a local ensemble transform Kalman filter is used. Compared to in situ observations, combining both methods led to the most significant improvements in the modeled concentrations and deposition, illustrating the usefulness of CrIS NH3 to improve the spatiotemporal distribution of NH3.
Abhinna K. Behera, Emmanuel D. Rivière, Sergey M. Khaykin, Virginie Marécal, Mélanie Ghysels, Jérémie Burgalat, and Gerhard Held
Atmos. Chem. Phys., 22, 881–901, https://doi.org/10.5194/acp-22-881-2022, https://doi.org/10.5194/acp-22-881-2022, 2022
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Deep convection overshooting the stratosphere's contribution to the global stratospheric water budget is still being quantified. We ran three different cloud-resolving simulations of an observed case of overshoots in Bauru during the TRO-Pico balloon campaign in the context of upscaling the impact of overshoots at a large scale. These simulations, which have been validated with balloon-borne and S-band radar measurements, shed light on the local-scale variability and composition of overshoots.
Cited articles
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Ayers, G. P., Gillett, R. W., Cainey, J. M., and Dick, A. L.: Chloride and bromide loss from sea-salt particles in Southern Ocean air, J. Atmos. Chem., 33, 299–319, https://doi.org/10.1023/A:1006120205159, 1999.
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