Articles | Volume 20, issue 14
https://doi.org/10.5194/acp-20-8405-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-20-8405-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Strong sensitivity of the isotopic composition of methane to the plausible range of tropospheric chlorine
Universities Space Research Association, Columbia, MD, USA
NASA Goddard Space Flight Center, Greenbelt, MD, USA
James S. Wang
Universities Space Research Association, Columbia, MD, USA
NASA Goddard Space Flight Center, Greenbelt, MD, USA
now at: Institute for Advanced Sustainability Studies,
Potsdam, Germany
Michael Manyin
NASA Goddard Space Flight Center, Greenbelt, MD, USA
Science Systems and Applications Inc. (SSAI), Lanham, MD, USA
Bryan Duncan
NASA Goddard Space Flight Center, Greenbelt, MD, USA
Ryan Hossaini
Lancaster Environment Centre, Lancaster University, Lancaster, UK
Christoph A. Keller
Universities Space Research Association, Columbia, MD, USA
NASA Goddard Space Flight Center, Greenbelt, MD, USA
Sylvia E. Michel
Institute of Arctic and Alpine Research, University of Colorado,
Boulder, Boulder, CO, USA
James W. C. White
Institute of Arctic and Alpine Research, University of Colorado,
Boulder, Boulder, CO, USA
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Irina Petropavlovskikh, Martine De Mazière, Anne M. Thompson, Jeannette D. Wild, James W. Hannigan, Henry B. Selkirk, Reem A. Hannun, Wolfgang Steinbrecht, Jean-Christopher Lambert, Roeland Van Malderen, Elizabeth Asher, Raul R. Cordero, Sophie Godin-Beekmann, Daan Hubert, Sergey Khaykin, Karin Kreher, Thierry Leblanc, Emmanuel Mahieu, Eliane Maillard Barras, Glen McConville, Gerald Nedoluha, Ivan Ortega, Alberto Redondas Marrero, Gunther Seckmeyer, Ryan M. Stauffer, Sarah A. Strode, Kim Strong, Takafumi Sugita, Michel Van Roozendael, Voltaire Velazco, Corinne Vigouroux, and Bärbel Vogel
Atmos. Chem. Phys., 26, 8637–8675, https://doi.org/10.5194/acp-26-8637-2026, https://doi.org/10.5194/acp-26-8637-2026, 2026
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This introduction to the special issue "Achievements and perspectives of the Network for the Detection of Atmospheric Composition Change after 35 years of operation” provides an overview of important research findings achieved under the NDACC objectives. The future of NDACC is discussed in the light of the evolution of the scientific questions, evolving collaborations with partners and Cooperating Networks, and the current landscape of gaps in satellite and ground-based observations.
Caterina Mogno, Peter R. Colarco, Allison B. Collow, Sampa Das, Sarah A. Strode, Vanessa Valenti, Michael E. Manyin, Qing Liang, Luke Oman, Stephen D. Steenrod, and K. Emma Knowland
Atmos. Chem. Phys., 26, 3025–3047, https://doi.org/10.5194/acp-26-3025-2026, https://doi.org/10.5194/acp-26-3025-2026, 2026
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We investigated a climate model's ability to simulate atmospheric aerosols focusing on the relationship between mass and optical properties, by comparing predictions with observations. Our analysis revealed that model errors in aerosol scattering primarily stem from inaccurate particle mass concentrations and relative humidity, rather than flawed optical property assumptions in the model. These findings point out improvements for enhancing the accuracy for aerosols representation in our model.
Huisheng Bian, Sarah Strode, Mian Chin, Fan Li, Andrea Molad, Peter R. Colarco, and Hongbin Yu
EGUsphere, https://doi.org/10.5194/egusphere-2025-4501, https://doi.org/10.5194/egusphere-2025-4501, 2025
Preprint archived
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We study the North Pacific westerly jet (NPWJ) using four reanalysis datasets and eight CMIP6 models. Our results show that between 1980 and 2019, the NPWJ core oscillates seasonally between north and south, weakening and shifting northward in summer and autumn. Single-forcing simulations further reveal aerosol forcing as the main driver. Incorporating interacting chemistry and time-varying ozone radiative forcing into Earth system models is crucial for simulating long-term atmospheric dynamics.
Bryan N. Duncan, Daniel C. Anderson, Arlene M. Fiore, Joanna Joiner, Nickolay A. Krotkov, Can Li, Dylan B. Millet, Julie M. Nicely, Luke D. Oman, Jason M. St. Clair, Joshua D. Shutter, Amir H. Souri, Sarah A. Strode, Brad Weir, Glenn M. Wolfe, Helen M. Worden, and Qindan Zhu
Atmos. Chem. Phys., 24, 13001–13023, https://doi.org/10.5194/acp-24-13001-2024, https://doi.org/10.5194/acp-24-13001-2024, 2024
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Trace gases emitted to or formed within the atmosphere may be chemically or physically removed from the atmosphere. One trace gas, the hydroxyl radical (OH), is responsible for initiating the chemical removal of many trace gases, including some greenhouse gases. Despite its importance, scientists have not been able to adequately measure OH. In this opinion piece, we discuss promising new methods to indirectly constrain OH using satellite data of trace gases that control the abundance of OH.
Yasin Elshorbany, Jerald R. Ziemke, Sarah Strode, Hervé Petetin, Kazuyuki Miyazaki, Isabelle De Smedt, Kenneth Pickering, Rodrigo J. Seguel, Helen Worden, Tamara Emmerichs, Domenico Taraborrelli, Maria Cazorla, Suvarna Fadnavis, Rebecca R. Buchholz, Benjamin Gaubert, Néstor Y. Rojas, Thiago Nogueira, Thérèse Salameh, and Min Huang
Atmos. Chem. Phys., 24, 12225–12257, https://doi.org/10.5194/acp-24-12225-2024, https://doi.org/10.5194/acp-24-12225-2024, 2024
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We investigated tropospheric ozone spatial variability and trends from 2005 to 2019 and related those to ozone precursors on global and regional scales. We also investigate the spatiotemporal characteristics of the ozone formation regime in relation to ozone chemical sources and sinks. Our analysis is based on remote sensing products of the tropospheric column of ozone and its precursors, nitrogen dioxide, formaldehyde, and total column CO, as well as ozonesonde data and model simulations.
Pinchas Nürnberg, Sarah A. Strode, and Ralf Sussmann
Atmos. Chem. Phys., 24, 10001–10012, https://doi.org/10.5194/acp-24-10001-2024, https://doi.org/10.5194/acp-24-10001-2024, 2024
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We created a set of scaling factors describing the diurnal increase in stratospheric nitrogen oxides above Zugspitze, Germany. We used these factors to validate recently published model simulation data. On the one hand, this validation enables the use of the validated data to better understand the stratospheric photochemistry. On the other hand, it can improve satellite validation, which has implications for the understanding of urban smog events and other pollution events in the troposphere.
Amir H. Souri, Bryan N. Duncan, Sarah A. Strode, Daniel C. Anderson, Michael E. Manyin, Junhua Liu, Luke D. Oman, Zhen Zhang, and Brad Weir
Atmos. Chem. Phys., 24, 8677–8701, https://doi.org/10.5194/acp-24-8677-2024, https://doi.org/10.5194/acp-24-8677-2024, 2024
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We explore a new method of using the wealth of information obtained from satellite observations of Aura OMI NO2, HCHO, and MERRA-2 reanalysis in NASA’s GEOS model equipped with an efficient tropospheric OH (TOH) estimator to enhance the representation of TOH spatial distribution and its long-term trends. This new framework helps us pinpoint regional inaccuracies in TOH and differentiate between established prior knowledge and newly acquired information from satellites on TOH trends.
Daniel C. Anderson, Bryan N. Duncan, Julie M. Nicely, Junhua Liu, Sarah A. Strode, and Melanie B. Follette-Cook
Atmos. Chem. Phys., 23, 6319–6338, https://doi.org/10.5194/acp-23-6319-2023, https://doi.org/10.5194/acp-23-6319-2023, 2023
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We describe a methodology that combines machine learning, satellite observations, and 3D chemical model output to infer the abundance of the hydroxyl radical (OH), a chemical that removes many trace gases from the atmosphere. The methodology successfully captures the variability of observed OH, although further observations are needed to evaluate absolute accuracy. Current satellite observations are of sufficient quality to infer OH, but retrieval validation in the remote tropics is needed.
Viral Shah, Daniel J. Jacob, Ruijun Dang, Lok N. Lamsal, Sarah A. Strode, Stephen D. Steenrod, K. Folkert Boersma, Sebastian D. Eastham, Thibaud M. Fritz, Chelsea Thompson, Jeff Peischl, Ilann Bourgeois, Ilana B. Pollack, Benjamin A. Nault, Ronald C. Cohen, Pedro Campuzano-Jost, Jose L. Jimenez, Simone T. Andersen, Lucy J. Carpenter, Tomás Sherwen, and Mat J. Evans
Atmos. Chem. Phys., 23, 1227–1257, https://doi.org/10.5194/acp-23-1227-2023, https://doi.org/10.5194/acp-23-1227-2023, 2023
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NOx in the free troposphere (above 2 km) affects global tropospheric chemistry and the retrieval and interpretation of satellite NO2 measurements. We evaluate free tropospheric NOx in global atmospheric chemistry models and find that recycling NOx from its reservoirs over the oceans is faster than that simulated in the models, resulting in increases in simulated tropospheric ozone and OH. Over the U.S., free tropospheric NO2 contributes the majority of the tropospheric NO2 column in summer.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven C. Wofsy
Atmos. Chem. Phys., 23, 99–117, https://doi.org/10.5194/acp-23-99-2023, https://doi.org/10.5194/acp-23-99-2023, 2023
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We have prepared a unique and unusual result from the recent ATom aircraft mission: a measurement-based derivation of the production and loss rates of ozone and methane over the ocean basins. These are the key products of chemistry models used in assessments but have thus far lacked observational metrics. It also shows the scales of variability of atmospheric chemical rates and provides a major challenge to the atmospheric models.
Sarah A. Strode, Ghassan Taha, Luke D. Oman, Robert Damadeo, David Flittner, Mark Schoeberl, Christopher E. Sioris, and Ryan Stauffer
Atmos. Meas. Tech., 15, 6145–6161, https://doi.org/10.5194/amt-15-6145-2022, https://doi.org/10.5194/amt-15-6145-2022, 2022
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We use a global atmospheric chemistry model simulation to generate scaling factors that account for the daily cycle of NO2 and ozone. These factors facilitate comparisons between sunrise and sunset observations from SAGE III/ISS and observations from other instruments. We provide the scaling factors as monthly zonal means for different latitudes and altitudes. We find that applying these factors yields more consistent comparisons between observations from SAGE III/ISS and other instruments.
Daniel C. Anderson, Melanie B. Follette-Cook, Sarah A. Strode, Julie M. Nicely, Junhua Liu, Peter D. Ivatt, and Bryan N. Duncan
Geosci. Model Dev., 15, 6341–6358, https://doi.org/10.5194/gmd-15-6341-2022, https://doi.org/10.5194/gmd-15-6341-2022, 2022
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The hydroxyl radical (OH) is the most important chemical in the atmosphere for removing certain pollutants, including methane, the second-most-important greenhouse gas. We present a methodology to create an easily modifiable parameterization that can calculate OH concentrations in a computationally efficient way. The parameterization, which predicts OH within 5 %, can be integrated into larger climate models to allow for calculation of the interactions between OH, methane, and other chemicals.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven Wofsy
Atmos. Chem. Phys., 21, 13729–13746, https://doi.org/10.5194/acp-21-13729-2021, https://doi.org/10.5194/acp-21-13729-2021, 2021
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The NASA Atmospheric Tomography (ATom) mission built a climatology of the chemical composition of tropospheric air parcels throughout the middle of the Pacific and Atlantic oceans. The level of detail allows us to reconstruct the photochemical budgets of O3 and CH4 over these vast, remote regions. We find that most of the chemical heterogeneity is captured at the resolution used in current global chemistry models and that the majority of reactivity occurs in the
hottest20 % of parcels.
Lucy Hart, Ryan Hossaini, Oliver Wild, Crispin Halsall, Martin K. Vollmer, and David Sherry
EGUsphere, https://doi.org/10.5194/egusphere-2026-4613, https://doi.org/10.5194/egusphere-2026-4613, 2026
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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HFO-1234yf is increasingly used in cars because of its low climate impact but once emitted to the atmosphere it forms trifluoroacetic acid (TFA), a chemical that remains on Earth permanently. We present the first global emission inventory of HFO-1234yf from cars and compare our results to atmospheric measurements. Using an atmospheric chemistry model, we found that TFA produced from this source is rapidly growing and most TFA is deposited outside of the region HFO-1234yf was emitted.
Irina Petropavlovskikh, Martine De Mazière, Anne M. Thompson, Jeannette D. Wild, James W. Hannigan, Henry B. Selkirk, Reem A. Hannun, Wolfgang Steinbrecht, Jean-Christopher Lambert, Roeland Van Malderen, Elizabeth Asher, Raul R. Cordero, Sophie Godin-Beekmann, Daan Hubert, Sergey Khaykin, Karin Kreher, Thierry Leblanc, Emmanuel Mahieu, Eliane Maillard Barras, Glen McConville, Gerald Nedoluha, Ivan Ortega, Alberto Redondas Marrero, Gunther Seckmeyer, Ryan M. Stauffer, Sarah A. Strode, Kim Strong, Takafumi Sugita, Michel Van Roozendael, Voltaire Velazco, Corinne Vigouroux, and Bärbel Vogel
Atmos. Chem. Phys., 26, 8637–8675, https://doi.org/10.5194/acp-26-8637-2026, https://doi.org/10.5194/acp-26-8637-2026, 2026
Short summary
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This introduction to the special issue "Achievements and perspectives of the Network for the Detection of Atmospheric Composition Change after 35 years of operation” provides an overview of important research findings achieved under the NDACC objectives. The future of NDACC is discussed in the light of the evolution of the scientific questions, evolving collaborations with partners and Cooperating Networks, and the current landscape of gaps in satellite and ground-based observations.
Bibhasvata Dasgupta, Sudhanshu Pandey, Sander Houweling, Malika Menoud, Carina van der Veen, John Miller, Ben Riddell-Young, Sylvia Englund Michel, Peter Sperlich, Shinji Morimoto, Ryo Fujita, Stephen Platt, Christine Groot Zwaaftink, Ingeborg Levin, Cordelia Veidt, Cathrine Lund Myhre, Ceres Woolley Maisch, Rebecca Fisher, Euan G. Nisbet, James France, Rowena Moss, Nicola Warwick, and Thomas Röckmann
Atmos. Chem. Phys., 26, 8601–8616, https://doi.org/10.5194/acp-26-8601-2026, https://doi.org/10.5194/acp-26-8601-2026, 2026
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Methane is a strong greenhouse gas, and its rise since the mid-2000s is debated in terms of sources and sinks. Using top-down and bottom-up data, along with inversion models and methane isotopes (δ13C-CH4 and δD-CH4), we find that wetlands are the primary driver of post-2006 increases, followed by agriculture and fossil fuels. Methane's lifetime has decreased by about 0.1 years. We also assess how isotope signatures and sink processes influence uncertainties.
Xuewei Hou, Ryan Hossaini, Oliver Wild, Andrea Mazzeo, Richard J. Pope, Ye Wang, Siyuan Wang, Yuanhong Zhao, James Lee, Bin Zhu, Tianliang Zhao, and Alok K. Pandey
EGUsphere, https://doi.org/10.5194/egusphere-2026-3114, https://doi.org/10.5194/egusphere-2026-3114, 2026
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The atmosphere’s ability to remove pollutants and greenhouse gases is largely controlled by the hydroxyl radical, but the causes of its long-term changes remain uncertain. Using a global atmospheric model, we quantified the effects of emissions, weather, and key chemical processes on hydroxyl radical levels between 2000 and 2017. Our findings improve understanding of atmospheric self-cleansing and help reduce uncertainties in future climate assessments.
Caterina Mogno, Peter R. Colarco, Allison B. Collow, Sampa Das, Sarah A. Strode, Vanessa Valenti, Michael E. Manyin, Qing Liang, Luke Oman, Stephen D. Steenrod, and K. Emma Knowland
Atmos. Chem. Phys., 26, 3025–3047, https://doi.org/10.5194/acp-26-3025-2026, https://doi.org/10.5194/acp-26-3025-2026, 2026
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We investigated a climate model's ability to simulate atmospheric aerosols focusing on the relationship between mass and optical properties, by comparing predictions with observations. Our analysis revealed that model errors in aerosol scattering primarily stem from inaccurate particle mass concentrations and relative humidity, rather than flawed optical property assumptions in the model. These findings point out improvements for enhancing the accuracy for aerosols representation in our model.
Amir H. Souri, Gonzalo González Abad, Bryan N. Duncan, and Luke D. Oman
Atmos. Chem. Phys., 26, 809–837, https://doi.org/10.5194/acp-26-809-2026, https://doi.org/10.5194/acp-26-809-2026, 2026
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We create long-term maps of PO3 magnitudes along with their corresponding sensitivity maps. This is achieved using a deep learning parameterization method that relies on satellite data, atmospheric models, and ground-based remote sensing. Our approach provides more quantitative information than commonly used methods that depend on ratio-based indicators (such as HCHO/NO2). Additionally, our method considers light and water vapor, making it suitable for applications with GEO satellites.
Bibhasvata Dasgupta, Malika Menoud, Carina van der Veen, Ingeborg Levin, Cordelia Veidt, Heiko Moossen, Sylvia Englund Michel, Peter Sperlich, Shinji Morimoto, Ryo Fujita, Taku Umezawa, Stephen Platt, Christine Groot Zwaaftink, Cathrine Lund Myhre, Rebecca Fisher, David Lowry, Euan G. Nisbet, James France, Ceres Woolley Maisch, Gordon Brailsford, Rowena Moss, Daisuke Goto, Sudhanshu Pandey, Sander Houweling, Nicola Warwick, and Thomas Röckmann
Atmos. Meas. Tech., 18, 6591–6607, https://doi.org/10.5194/amt-18-6591-2025, https://doi.org/10.5194/amt-18-6591-2025, 2025
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We combined long-term methane mole fraction and isotope measurements from eight laboratories that sample high-latitude stations to compare, offset correct and harmonise the datasets into a hemisphere merged timeseries. Because each laboratory uses slightly different methods, we adjusted the data to make it directly comparable. This allowed us to create a consistent record of atmospheric methane concentration and its isotopes from 1988 to 2023.
Huisheng Bian, Sarah Strode, Mian Chin, Fan Li, Andrea Molad, Peter R. Colarco, and Hongbin Yu
EGUsphere, https://doi.org/10.5194/egusphere-2025-4501, https://doi.org/10.5194/egusphere-2025-4501, 2025
Preprint archived
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We study the North Pacific westerly jet (NPWJ) using four reanalysis datasets and eight CMIP6 models. Our results show that between 1980 and 2019, the NPWJ core oscillates seasonally between north and south, weakening and shifting northward in summer and autumn. Single-forcing simulations further reveal aerosol forcing as the main driver. Incorporating interacting chemistry and time-varying ozone radiative forcing into Earth system models is crucial for simulating long-term atmospheric dynamics.
Yunqian Zhu, Hideharu Akiyoshi, Valentina Aquila, Elizabeth Asher, Ewa M. Bednarz, Slimane Bekki, Christoph Brühl, Amy H. Butler, Parker Case, Simon Chabrillat, Gabriel Chiodo, Margot Clyne, Peter R. Colarco, Sandip Dhomse, Lola Falletti, Eric Fleming, Ben Johnson, Andrin Jörimann, Mahesh Kovilakam, Gerbrand Koren, Ales Kuchar, Nicolas Lebas, Qing Liang, Cheng-Cheng Liu, Graham Mann, Michael Manyin, Marion Marchand, Olaf Morgenstern, Paul Newman, Luke D. Oman, Freja F. Østerstrøm, Yifeng Peng, David Plummer, Ilaria Quaglia, William Randel, Samuel Rémy, Takashi Sekiya, Stephen Steenrod, Timofei Sukhodolov, Simone Tilmes, Kostas Tsigaridis, Rei Ueyama, Daniele Visioni, Xinyue Wang, Shingo Watanabe, Yousuke Yamashita, Pengfei Yu, Wandi Yu, Jun Zhang, and Zhihong Zhuo
Geosci. Model Dev., 18, 5487–5512, https://doi.org/10.5194/gmd-18-5487-2025, https://doi.org/10.5194/gmd-18-5487-2025, 2025
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To understand the climate impact of the 2022 Hunga volcanic eruption, we developed a climate model–observation comparison project. The paper describes the protocols and models that participate in the experiments. We designed several experiments to achieve our goals of this activity: (1) to evaluate the climate model performance and (2) to understand the Earth system responses to this eruption.
Meghana Velagar, Christoph Keller, and J. Nathan Kutz
Geosci. Model Dev., 18, 4667–4684, https://doi.org/10.5194/gmd-18-4667-2025, https://doi.org/10.5194/gmd-18-4667-2025, 2025
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We develop the data-driven method of dynamic mode decomposition for producing a robust and stable surrogate reduced-order model of atmospheric chemistry dynamics. The model is computationally efficient, provides interpretable patterns of activity, and produces uncertainty quantification metrics. It is ideal for the forecasting of atmospheric chemistry in a computationally tractable manner.
Alok K. Pandey, David S. Stevenson, Alcide Zhao, Richard J. Pope, Ryan Hossaini, Krishan Kumar, and Martyn P. Chipperfield
Atmos. Chem. Phys., 25, 4785–4802, https://doi.org/10.5194/acp-25-4785-2025, https://doi.org/10.5194/acp-25-4785-2025, 2025
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Nitrogen dioxide is an air pollutant largely controlled by human activity that affects ozone, methane, and aerosols. Satellite instruments can quantify column NO2 and, by carefully matching the time and location of measurements, enable evaluation of model simulations. NO2 over south and east Asia is assessed, showing that the model captures not only many features of the measurements, but also important differences that suggest model deficiencies in representing several aspects of the atmospheric chemistry of NO2.
Hongyu Liu, Bo Zhang, Richard H. Moore, Luke D. Ziemba, Richard A. Ferrare, Hyundeok Choi, Armin Sorooshian, David Painemal, Hailong Wang, Michael A. Shook, Amy Jo Scarino, Johnathan W. Hair, Ewan C. Crosbie, Marta A. Fenn, Taylor J. Shingler, Chris A. Hostetler, Gao Chen, Mary M. Kleb, Gan Luo, Fangqun Yu, Mark A. Vaughan, Yongxiang Hu, Glenn S. Diskin, John B. Nowak, Joshua P. DiGangi, Yonghoon Choi, Christoph A. Keller, and Matthew S. Johnson
Atmos. Chem. Phys., 25, 2087–2121, https://doi.org/10.5194/acp-25-2087-2025, https://doi.org/10.5194/acp-25-2087-2025, 2025
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We use the GEOS-Chem model to simulate aerosol distributions and properties over the western North Atlantic Ocean (WNAO) during the winter and summer deployments in 2020 of the NASA ACTIVATE mission. Model results are evaluated against aircraft, ground-based, and satellite observations. The improved understanding of life cycle, composition, transport pathways, and distribution of aerosols has important implications for characterizing aerosol–cloud–meteorology interactions over WNAO.
Amir H. Souri, Gonzalo González Abad, Glenn M. Wolfe, Tijl Verhoelst, Corinne Vigouroux, Gaia Pinardi, Steven Compernolle, Bavo Langerock, Bryan N. Duncan, and Matthew S. Johnson
Atmos. Chem. Phys., 25, 2061–2086, https://doi.org/10.5194/acp-25-2061-2025, https://doi.org/10.5194/acp-25-2061-2025, 2025
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We establish a simple yet robust relationship between ozone production rates and geophysical parameters obtained from several intensive atmospheric composition campaigns. We show that satellite remote sensing data can effectively constrain these parameters, enabling us to produce the first global maps of ozone production rates with unprecedented resolution.
Ryan Hossaini, David Sherry, Zihao Wang, Martyn P. Chipperfield, Wuhu Feng, David E. Oram, Karina E. Adcock, Stephen A. Montzka, Isobel J. Simpson, Andrea Mazzeo, Amber A. Leeson, Elliot Atlas, and Charles C.-K. Chou
Atmos. Chem. Phys., 24, 13457–13475, https://doi.org/10.5194/acp-24-13457-2024, https://doi.org/10.5194/acp-24-13457-2024, 2024
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DCE (1,2-dichloroethane) is an industrial chemical used to produce PVC (polyvinyl chloride). We analysed DCE production data to estimate global DCE emissions (2002–2020). The emissions were included in an atmospheric model and evaluated by comparing simulated DCE to DCE measurements in the troposphere. We show that DCE contributes ozone-depleting Cl to the stratosphere and that this has increased with increasing DCE emissions. DCE’s impact on stratospheric O3 is currently small but non-zero.
Bryan N. Duncan, Daniel C. Anderson, Arlene M. Fiore, Joanna Joiner, Nickolay A. Krotkov, Can Li, Dylan B. Millet, Julie M. Nicely, Luke D. Oman, Jason M. St. Clair, Joshua D. Shutter, Amir H. Souri, Sarah A. Strode, Brad Weir, Glenn M. Wolfe, Helen M. Worden, and Qindan Zhu
Atmos. Chem. Phys., 24, 13001–13023, https://doi.org/10.5194/acp-24-13001-2024, https://doi.org/10.5194/acp-24-13001-2024, 2024
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Trace gases emitted to or formed within the atmosphere may be chemically or physically removed from the atmosphere. One trace gas, the hydroxyl radical (OH), is responsible for initiating the chemical removal of many trace gases, including some greenhouse gases. Despite its importance, scientists have not been able to adequately measure OH. In this opinion piece, we discuss promising new methods to indirectly constrain OH using satellite data of trace gases that control the abundance of OH.
Yasin Elshorbany, Jerald R. Ziemke, Sarah Strode, Hervé Petetin, Kazuyuki Miyazaki, Isabelle De Smedt, Kenneth Pickering, Rodrigo J. Seguel, Helen Worden, Tamara Emmerichs, Domenico Taraborrelli, Maria Cazorla, Suvarna Fadnavis, Rebecca R. Buchholz, Benjamin Gaubert, Néstor Y. Rojas, Thiago Nogueira, Thérèse Salameh, and Min Huang
Atmos. Chem. Phys., 24, 12225–12257, https://doi.org/10.5194/acp-24-12225-2024, https://doi.org/10.5194/acp-24-12225-2024, 2024
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We investigated tropospheric ozone spatial variability and trends from 2005 to 2019 and related those to ozone precursors on global and regional scales. We also investigate the spatiotemporal characteristics of the ozone formation regime in relation to ozone chemical sources and sinks. Our analysis is based on remote sensing products of the tropospheric column of ozone and its precursors, nitrogen dioxide, formaldehyde, and total column CO, as well as ozonesonde data and model simulations.
Pinchas Nürnberg, Sarah A. Strode, and Ralf Sussmann
Atmos. Chem. Phys., 24, 10001–10012, https://doi.org/10.5194/acp-24-10001-2024, https://doi.org/10.5194/acp-24-10001-2024, 2024
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We created a set of scaling factors describing the diurnal increase in stratospheric nitrogen oxides above Zugspitze, Germany. We used these factors to validate recently published model simulation data. On the one hand, this validation enables the use of the validated data to better understand the stratospheric photochemistry. On the other hand, it can improve satellite validation, which has implications for the understanding of urban smog events and other pollution events in the troposphere.
Amir H. Souri, Bryan N. Duncan, Sarah A. Strode, Daniel C. Anderson, Michael E. Manyin, Junhua Liu, Luke D. Oman, Zhen Zhang, and Brad Weir
Atmos. Chem. Phys., 24, 8677–8701, https://doi.org/10.5194/acp-24-8677-2024, https://doi.org/10.5194/acp-24-8677-2024, 2024
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We explore a new method of using the wealth of information obtained from satellite observations of Aura OMI NO2, HCHO, and MERRA-2 reanalysis in NASA’s GEOS model equipped with an efficient tropospheric OH (TOH) estimator to enhance the representation of TOH spatial distribution and its long-term trends. This new framework helps us pinpoint regional inaccuracies in TOH and differentiate between established prior knowledge and newly acquired information from satellites on TOH trends.
Lily Gouldsbrough, Ryan Hossaini, Emma Eastoe, Paul J. Young, and Massimo Vieno
Atmos. Chem. Phys., 24, 3163–3196, https://doi.org/10.5194/acp-24-3163-2024, https://doi.org/10.5194/acp-24-3163-2024, 2024
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High-resolution spatial fields of surface ozone are used to understand spikes in ozone concentration and predict their impact on public health. Such fields are routinely output from complex mathematical models for atmospheric conditions. These outputs are on a coarse spatial resolution and the highest concentrations tend to be biased. Using a novel data-driven machine learning methodology, we show how such output can be corrected to produce fields with both lower bias and higher resolution.
Douglas E. J. Worthy, Michele K. Rauh, Lin Huang, Felix R. Vogel, Alina Chivulescu, Kenneth A. Masarie, Ray L. Langenfelds, Paul B. Krummel, Colin E. Allison, Andrew M. Crotwell, Monica Madronich, Gabrielle Pétron, Ingeborg Levin, Samuel Hammer, Sylvia Michel, Michel Ramonet, Martina Schmidt, Armin Jordan, Heiko Moossen, Michael Rothe, Ralph Keeling, and Eric J. Morgan
Atmos. Meas. Tech., 16, 5909–5935, https://doi.org/10.5194/amt-16-5909-2023, https://doi.org/10.5194/amt-16-5909-2023, 2023
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Network compatibility is important for inferring greenhouse gas fluxes at global or regional scales. This study is the first assessment of the measurement agreement among seven individual programs within the World Meteorological Organization community. It compares co-located flask air measurements at the Alert Observatory in Canada over a 17-year period. The results provide stronger confidence in the uncertainty estimation while using those datasets in various data interpretation applications.
Jinsol Kim, John B. Miller, Charles E. Miller, Scott J. Lehman, Sylvia E. Michel, Vineet Yadav, Nick E. Rollins, and William M. Berelson
Atmos. Chem. Phys., 23, 14425–14436, https://doi.org/10.5194/acp-23-14425-2023, https://doi.org/10.5194/acp-23-14425-2023, 2023
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In this study, we present the partitioning of CO2 signals from biogenic, petroleum and natural gas sources by combining CO, 13CO2 and 14CO2 measurements. Using measurements from flask air samples at three sites in the greater Los Angeles region, we find larger and positive contributions of biogenic signals in winter and smaller and negative contributions in summer. The largest contribution of natural gas combustion generally occurs in summer.
Ewa M. Bednarz, Ryan Hossaini, and Martyn P. Chipperfield
Atmos. Chem. Phys., 23, 13701–13711, https://doi.org/10.5194/acp-23-13701-2023, https://doi.org/10.5194/acp-23-13701-2023, 2023
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We quantify, for the first time, the time-varying impact of uncontrolled emissions of chlorinated very short-lived substances (Cl-VSLSs) on stratospheric ozone using a state-of-the-art chemistry-climate model. We demonstrate that Cl-VSLSs already have a non-negligible impact on stratospheric ozone, including a local reduction of up to ~7 DU in Arctic ozone in the cold winter of 2019/20, and any so future growth in emissions will continue to offset some of the benefits of the Montreal Protocol.
Ewa M. Bednarz, Ryan Hossaini, N. Luke Abraham, and Martyn P. Chipperfield
Geosci. Model Dev., 16, 6187–6209, https://doi.org/10.5194/gmd-16-6187-2023, https://doi.org/10.5194/gmd-16-6187-2023, 2023
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Development and performance of the new DEST chemistry scheme of UM–UKCA is described. The scheme extends the standard StratTrop scheme by including important updates to the halogen chemistry, thus allowing process-oriented studies of stratospheric ozone depletion and recovery, including impacts from both controlled long-lived ozone-depleting substances and emerging issues around uncontrolled, very short-lived substances. It will thus aid studies in support of future ozone assessment reports.
Alice Drinkwater, Paul I. Palmer, Liang Feng, Tim Arnold, Xin Lan, Sylvia E. Michel, Robert Parker, and Hartmut Boesch
Atmos. Chem. Phys., 23, 8429–8452, https://doi.org/10.5194/acp-23-8429-2023, https://doi.org/10.5194/acp-23-8429-2023, 2023
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Changes in atmospheric methane over the last few decades are largely unexplained. Previous studies have proposed different hypotheses to explain short-term changes in atmospheric methane. We interpret observed changes in atmospheric methane and stable isotope source signatures (2004–2020). We argue that changes over this period are part of a large-scale shift from high-northern-latitude thermogenic energy emissions to tropical biogenic emissions, particularly from North Africa and South America.
Daniel C. Anderson, Bryan N. Duncan, Julie M. Nicely, Junhua Liu, Sarah A. Strode, and Melanie B. Follette-Cook
Atmos. Chem. Phys., 23, 6319–6338, https://doi.org/10.5194/acp-23-6319-2023, https://doi.org/10.5194/acp-23-6319-2023, 2023
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We describe a methodology that combines machine learning, satellite observations, and 3D chemical model output to infer the abundance of the hydroxyl radical (OH), a chemical that removes many trace gases from the atmosphere. The methodology successfully captures the variability of observed OH, although further observations are needed to evaluate absolute accuracy. Current satellite observations are of sufficient quality to infer OH, but retrieval validation in the remote tropics is needed.
Viral Shah, Daniel J. Jacob, Ruijun Dang, Lok N. Lamsal, Sarah A. Strode, Stephen D. Steenrod, K. Folkert Boersma, Sebastian D. Eastham, Thibaud M. Fritz, Chelsea Thompson, Jeff Peischl, Ilann Bourgeois, Ilana B. Pollack, Benjamin A. Nault, Ronald C. Cohen, Pedro Campuzano-Jost, Jose L. Jimenez, Simone T. Andersen, Lucy J. Carpenter, Tomás Sherwen, and Mat J. Evans
Atmos. Chem. Phys., 23, 1227–1257, https://doi.org/10.5194/acp-23-1227-2023, https://doi.org/10.5194/acp-23-1227-2023, 2023
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NOx in the free troposphere (above 2 km) affects global tropospheric chemistry and the retrieval and interpretation of satellite NO2 measurements. We evaluate free tropospheric NOx in global atmospheric chemistry models and find that recycling NOx from its reservoirs over the oceans is faster than that simulated in the models, resulting in increases in simulated tropospheric ozone and OH. Over the U.S., free tropospheric NO2 contributes the majority of the tropospheric NO2 column in summer.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven C. Wofsy
Atmos. Chem. Phys., 23, 99–117, https://doi.org/10.5194/acp-23-99-2023, https://doi.org/10.5194/acp-23-99-2023, 2023
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We have prepared a unique and unusual result from the recent ATom aircraft mission: a measurement-based derivation of the production and loss rates of ozone and methane over the ocean basins. These are the key products of chemistry models used in assessments but have thus far lacked observational metrics. It also shows the scales of variability of atmospheric chemical rates and provides a major challenge to the atmospheric models.
Sourish Basu, Xin Lan, Edward Dlugokencky, Sylvia Michel, Stefan Schwietzke, John B. Miller, Lori Bruhwiler, Youmi Oh, Pieter P. Tans, Francesco Apadula, Luciana V. Gatti, Armin Jordan, Jaroslaw Necki, Motoki Sasakawa, Shinji Morimoto, Tatiana Di Iorio, Haeyoung Lee, Jgor Arduini, and Giovanni Manca
Atmos. Chem. Phys., 22, 15351–15377, https://doi.org/10.5194/acp-22-15351-2022, https://doi.org/10.5194/acp-22-15351-2022, 2022
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Atmospheric methane (CH4) has been growing steadily since 2007 for reasons that are not well understood. Here we determine sources of methane using a technique informed by atmospheric measurements of CH4 and its isotopologue 13CH4. Measurements of 13CH4 provide for better separation of microbial, fossil, and fire sources of methane than CH4 measurements alone. Compared to previous assessments such as the Global Carbon Project, we find a larger microbial contribution to the post-2007 increase.
Randall V. Martin, Sebastian D. Eastham, Liam Bindle, Elizabeth W. Lundgren, Thomas L. Clune, Christoph A. Keller, William Downs, Dandan Zhang, Robert A. Lucchesi, Melissa P. Sulprizio, Robert M. Yantosca, Yanshun Li, Lucas Estrada, William M. Putman, Benjamin M. Auer, Atanas L. Trayanov, Steven Pawson, and Daniel J. Jacob
Geosci. Model Dev., 15, 8731–8748, https://doi.org/10.5194/gmd-15-8731-2022, https://doi.org/10.5194/gmd-15-8731-2022, 2022
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Atmospheric chemistry models must be able to operate both online as components of Earth system models and offline as standalone models. The widely used GEOS-Chem model operates both online and offline, but the classic offline version is not suitable for massively parallel simulations. We describe a new generation of the offline high-performance GEOS-Chem (GCHP) that enables high-resolution simulations on thousands of cores, including on the cloud, with improved access, performance, and accuracy.
Markus Jesswein, Rafael P. Fernandez, Lucas Berná, Alfonso Saiz-Lopez, Jens-Uwe Grooß, Ryan Hossaini, Eric C. Apel, Rebecca S. Hornbrook, Elliot L. Atlas, Donald R. Blake, Stephen Montzka, Timo Keber, Tanja Schuck, Thomas Wagenhäuser, and Andreas Engel
Atmos. Chem. Phys., 22, 15049–15070, https://doi.org/10.5194/acp-22-15049-2022, https://doi.org/10.5194/acp-22-15049-2022, 2022
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This study presents the global and seasonal distribution of the two major brominated short-lived substances CH2Br2 and CHBr3 in the upper troposphere and lower stratosphere based on observations from several aircraft campaigns. They show similar seasonality for both hemispheres, except in the respective hemispheric autumn lower stratosphere. A comparison with the TOMCAT and CAM-Chem models shows good agreement in the annual mean but larger differences in the seasonal consideration.
Sarah A. Strode, Ghassan Taha, Luke D. Oman, Robert Damadeo, David Flittner, Mark Schoeberl, Christopher E. Sioris, and Ryan Stauffer
Atmos. Meas. Tech., 15, 6145–6161, https://doi.org/10.5194/amt-15-6145-2022, https://doi.org/10.5194/amt-15-6145-2022, 2022
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We use a global atmospheric chemistry model simulation to generate scaling factors that account for the daily cycle of NO2 and ozone. These factors facilitate comparisons between sunrise and sunset observations from SAGE III/ISS and observations from other instruments. We provide the scaling factors as monthly zonal means for different latitudes and altitudes. We find that applying these factors yields more consistent comparisons between observations from SAGE III/ISS and other instruments.
Ewa M. Bednarz, Ryan Hossaini, Martyn P. Chipperfield, N. Luke Abraham, and Peter Braesicke
Atmos. Chem. Phys., 22, 10657–10676, https://doi.org/10.5194/acp-22-10657-2022, https://doi.org/10.5194/acp-22-10657-2022, 2022
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Atmospheric impacts of chlorinated very short-lived substances (Cl-VSLS) over the first two decades of the 21st century are assessed using the UM-UKCA chemistry–climate model. Stratospheric input of Cl from Cl-VSLS is estimated at ~130 ppt in 2019. The use of model set-up with constrained meteorology significantly increases the abundance of Cl-VSLS in the lower stratosphere relative to the free-running set-up. The growth in Cl-VSLS emissions significantly impacted recent HCl and COCl2 trends.
Daniel C. Anderson, Melanie B. Follette-Cook, Sarah A. Strode, Julie M. Nicely, Junhua Liu, Peter D. Ivatt, and Bryan N. Duncan
Geosci. Model Dev., 15, 6341–6358, https://doi.org/10.5194/gmd-15-6341-2022, https://doi.org/10.5194/gmd-15-6341-2022, 2022
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The hydroxyl radical (OH) is the most important chemical in the atmosphere for removing certain pollutants, including methane, the second-most-important greenhouse gas. We present a methodology to create an easily modifiable parameterization that can calculate OH concentrations in a computationally efficient way. The parameterization, which predicts OH within 5 %, can be integrated into larger climate models to allow for calculation of the interactions between OH, methane, and other chemicals.
Joël Thanwerdas, Marielle Saunois, Antoine Berchet, Isabelle Pison, Bruce H. Vaughn, Sylvia Englund Michel, and Philippe Bousquet
Geosci. Model Dev., 15, 4831–4851, https://doi.org/10.5194/gmd-15-4831-2022, https://doi.org/10.5194/gmd-15-4831-2022, 2022
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Estimating CH4 sources by exploiting observations within an inverse modeling framework is a powerful approach. Here, a new system designed to assimilate δ13C(CH4) observations together with CH4 observations is presented. By optimizing both the emissions and associated source signatures of multiple emission categories, this new system can efficiently differentiate the co-located emission categories and provide estimates of CH4 sources that are consistent with isotopic data.
Eric Saboya, Giulia Zazzeri, Heather Graven, Alistair J. Manning, and Sylvia Englund Michel
Atmos. Chem. Phys., 22, 3595–3613, https://doi.org/10.5194/acp-22-3595-2022, https://doi.org/10.5194/acp-22-3595-2022, 2022
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Continuous measurements of atmospheric methane concentrations and its carbon-13 isotope have been made in central London since early 2018. These measurements were used to evaluate methane emissions reported in global and UK-specific emission inventories for the London area. Compared to atmospheric methane measurements from March 2018 to October 2020, both inventories are under-reporting natural gas leakage for the London area.
Sandip S. Dhomse, Martyn P. Chipperfield, Wuhu Feng, Ryan Hossaini, Graham W. Mann, Michelle L. Santee, and Mark Weber
Atmos. Chem. Phys., 22, 903–916, https://doi.org/10.5194/acp-22-903-2022, https://doi.org/10.5194/acp-22-903-2022, 2022
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Solar flux variations associated with 11-year sunspot cycle is believed to exert important external climate forcing. As largest variations occur at shorter wavelengths such as ultra-violet part of the solar spectrum, associated changes in stratospheric ozone are thought to provide direct evidence for solar climate interaction. Until now, most of the studies reported double-peak structured solar cycle signal (SCS), but relatively new satellite data suggest only single-peak-structured SCS.
Paul D. Hamer, Virginie Marécal, Ryan Hossaini, Michel Pirre, Gisèle Krysztofiak, Franziska Ziska, Andreas Engel, Stephan Sala, Timo Keber, Harald Bönisch, Elliot Atlas, Kirstin Krüger, Martyn Chipperfield, Valery Catoire, Azizan A. Samah, Marcel Dorf, Phang Siew Moi, Hans Schlager, and Klaus Pfeilsticker
Atmos. Chem. Phys., 21, 16955–16984, https://doi.org/10.5194/acp-21-16955-2021, https://doi.org/10.5194/acp-21-16955-2021, 2021
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Bromoform is a stratospheric ozone-depleting gas released by seaweed and plankton transported to the stratosphere via convection in the tropics. We study the chemical interactions of bromoform and its derivatives within convective clouds using a cloud-scale model and observations. Our findings are that soluble bromine gases are efficiently washed out and removed within the convective clouds and that most bromine is transported vertically to the upper troposphere in the form of bromoform.
Vilma Kangasaho, Aki Tsuruta, Leif Backman, Pyry Mäkinen, Sander Houweling, Arjo Segers, Maarten Krol, Ed Dlugokencky, Sylvia Michel, James White, and Tuula Aalto
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-843, https://doi.org/10.5194/acp-2021-843, 2021
Revised manuscript not accepted
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Understanding the composition of carbon isotopes can help to better understand the changes in methane budgets. This study investigates how methane sources affect the seasonal cycle of the methane carbon-13 isotope during 2000–2012 using an atmospheric transport model. We found that emissions from both anthropogenic and natural sources contribute. The findings raise a need to revise the magnitudes, proportion, and seasonal cycles of anthropogenic sources and northern wetland emissions.
Abigail G. Hughes, Sonja Wahl, Tyler R. Jones, Alexandra Zuhr, Maria Hörhold, James W. C. White, and Hans Christian Steen-Larsen
The Cryosphere, 15, 4949–4974, https://doi.org/10.5194/tc-15-4949-2021, https://doi.org/10.5194/tc-15-4949-2021, 2021
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Water isotope records in Greenland and Antarctic ice cores are a valuable proxy for paleoclimate reconstruction and are traditionally thought to primarily reflect precipitation input. However,
post-depositional processes are hypothesized to contribute to the isotope climate signal. In this study we use laboratory experiments, field experiments, and modeling to show that sublimation and vapor–snow isotope exchange can rapidly influence the isotopic composition of the snowpack.
Liam Bindle, Randall V. Martin, Matthew J. Cooper, Elizabeth W. Lundgren, Sebastian D. Eastham, Benjamin M. Auer, Thomas L. Clune, Hongjian Weng, Jintai Lin, Lee T. Murray, Jun Meng, Christoph A. Keller, William M. Putman, Steven Pawson, and Daniel J. Jacob
Geosci. Model Dev., 14, 5977–5997, https://doi.org/10.5194/gmd-14-5977-2021, https://doi.org/10.5194/gmd-14-5977-2021, 2021
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Atmospheric chemistry models like GEOS-Chem are versatile tools widely used in air pollution and climate studies. The simulations used in such studies can be very computationally demanding, and thus it is useful if the model can simulate a specific geographic region at a higher resolution than the rest of the globe. Here, we implement, test, and demonstrate a new variable-resolution capability in GEOS-Chem that is suitable for simulations conducted on supercomputers.
Huisheng Bian, Eunjee Lee, Randal D. Koster, Donifan Barahona, Mian Chin, Peter R. Colarco, Anton Darmenov, Sarith Mahanama, Michael Manyin, Peter Norris, John Shilling, Hongbin Yu, and Fanwei Zeng
Atmos. Chem. Phys., 21, 14177–14197, https://doi.org/10.5194/acp-21-14177-2021, https://doi.org/10.5194/acp-21-14177-2021, 2021
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The study using the NASA Earth system model shows ~2.6 % increase in burning season gross primary production and ~1.5 % increase in annual net primary production across the Amazon Basin during 2010–2016 due to the change in surface downward direct and diffuse photosynthetically active radiation by biomass burning aerosols. Such an aerosol effect is strongly dependent on the presence of clouds. The cloud fraction at which aerosols switch from stimulating to inhibiting plant growth occurs at ~0.8.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven Wofsy
Atmos. Chem. Phys., 21, 13729–13746, https://doi.org/10.5194/acp-21-13729-2021, https://doi.org/10.5194/acp-21-13729-2021, 2021
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The NASA Atmospheric Tomography (ATom) mission built a climatology of the chemical composition of tropospheric air parcels throughout the middle of the Pacific and Atlantic oceans. The level of detail allows us to reconstruct the photochemical budgets of O3 and CH4 over these vast, remote regions. We find that most of the chemical heterogeneity is captured at the resolution used in current global chemistry models and that the majority of reactivity occurs in the
hottest20 % of parcels.
Haipeng Lin, Daniel J. Jacob, Elizabeth W. Lundgren, Melissa P. Sulprizio, Christoph A. Keller, Thibaud M. Fritz, Sebastian D. Eastham, Louisa K. Emmons, Patrick C. Campbell, Barry Baker, Rick D. Saylor, and Raffaele Montuoro
Geosci. Model Dev., 14, 5487–5506, https://doi.org/10.5194/gmd-14-5487-2021, https://doi.org/10.5194/gmd-14-5487-2021, 2021
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Emissions are a central component of atmospheric chemistry models. The Harmonized Emissions Component (HEMCO) is a software component for computing emissions from a user-selected ensemble of emission inventories and algorithms. It allows users to select, add, and scale emissions from different sources through a configuration file with no change to the model source code. We demonstrate the implementation of HEMCO in several models, all sharing the same HEMCO core code and database library.
Cited articles
Allan, W., Manning, M. R., Lassey, K. R., Lowe, D. C., and Gomez, A. J.:
Modeling the variation of δ13C in atmospheric methane: Phase
ellipses and the kinetic isotope effect, Global Biogeochem. Cy., 15,
467–481, https://doi.org/10.1029/2000GB001282, 2001.
Allan, W., Struthers, H., and Lowe, D.: Methane carbon isotope effects
caused by atomic chlorine in the marine boundary layer: Global model results
compared with Southern Hemisphere measurements, J. Geophys.
Res.-Atmos., 112, D04306, https://doi.org/10.1029/2006JD007369, 2007.
Bock, M., Schmitt, J., Beck, J., Seth, B., Chappellaz, J., and Fischer, H.:
Glacial/interglacial wetland, biomass burning, and geologic methane
emissions constrained by dual stable isotopic CH4 ice core records,
P. Natl. Acad. Sci. USA, 114, E5778–E5786,
https://doi.org/10.1073/pnas.1613883114, 2017.
Brownlow, R., Lowry, D., Fisher, R., France, J., Lanoisellé, M., White,
B., Wooster, M., Zhang, T., and Nisbet, E.: Isotopic ratios of tropical
methane emissions by atmospheric measurement, Global Biogeochem. Cy.,
31, 1408–1419, 2017.
Cantrell, C. A., Shetter, R. E., McDaniel, A. H., Calvert, J. G., Davidson,
J. A., Lowe, D. C., Tyler, S. C., Cicerone, R. J., and Greenberg, J. P.:
Carbon kinetic isotope effect in the oxidation of methane by the hydroxyl
radical, J. Geophys. Res.-Atmos., 95, 22455–22462,
1990.
Craig, H.: Isotopic Standards for Carbon and Oxygen and Correction Factors
for Mass-Spectrometric Analysis OF Carbon Dioxide, Geochim.
Cosmochim. Ac., 12, 133–149, https://doi.org/10.1016/0016-7037(57)90024-8, 1957.
Dlugokencky, E., Bruhwiler, L., White, J., Emmons, L., Novelli, P., Montzka,
S., Masarie, K., Lang, P., Crotwell, A., Miller, J., and Gatti, L.:
Observational constraints on recent increases in the atmospheric CH4 burden,
Geophys. Res. Lett., 36, L18803, https://doi.org/10.1029/2009GL039780, 2009.
Dlugokencky, E., Nisbet, E., Fisher, R., and Lowry, D.: Global atmospheric
methane: budget, changes and dangers, Philos. T.
R. Soc. A, 369,
2058–2072, https://doi.org/10.1098/rsta.2010.0341, 2011.
Dlugokencky, E. J., Lang, P. M., Crotwell, A. M., Mund, J. W., Crotwell, M. J., and
Thoning, K. W.: Atmospheric Methane Dry Air Mole Fractions from the NOAA ESRL
Carbon Cycle Cooperative Global Air Sampling Network, 1983–2017, Version:
2018-08-01, available at: ftp://aftp.cmdl.noaa.gov/data/trace_gases/ch4/flask/surface/ (last access: 30 January 2019), 2018.
Duncan, B. N., Strahan, S. E., Yoshida, Y., Steenrod, S. D., and Livesey, N.: Model study of the cross-tropopause transport of biomass burning pollution, Atmos. Chem. Phys., 7, 3713–3736, https://doi.org/10.5194/acp-7-3713-2007, 2007.
Elshorbany, Y. F., Duncan, B. N., Strode, S. A., Wang, J. S., and Kouatchou, J.: The description and validation of the computationally Efficient CH4–CO–OH (ECCOHv1.01) chemistry module for 3-D model applications, Geosci. Model Dev., 9, 799–822, https://doi.org/10.5194/gmd-9-799-2016, 2016.
Etiope, G. and Milkov, A.: A new estimate of global methane flux from
onshore and shallow submarine mud volcanoes to the atmosphere, Environ.
Geol., 46, 997–1002, https://doi.org/10.1007/s00254-004-1085-1, 2004.
European Commission: Joint Research Center (JRC)/Netherlands Environmental
Assessment Agency (PBL), Emission Database for Global Atmospheric Research
(EDGAR), available at: http://edgar.jrc.ec.europe.eu (last access: 6 July 2016), 2011.
Ferretti, D. F., Miller, J. B., White, J. W. C., Etheridge, D. M., Lassey,
K. R., Lowe, D. C., Meure, C. M. M., Dreier, M. F., Trudinger, C. M., van
Ommen, T. D., and Langenfelds, R. L.: Unexpected Changes to the Global
Methane Budget over the Past 2000 Years, Science, 309, 1714–1717,
https://doi.org/10.1126/science.1115193, 2005.
Fischer, H., Behrens, M., Bock, M., Richter, U., Schmitt, J., Loulergue, L.,
Chappellaz, J., Spahni, R., Blunier, T., Leuenberger, M., and Stocker, T.
F.: Changing boreal methane sources and constant biomass burning during the
last termination, Nature, 452, 864, https://doi.org/10.1038/nature06825,
2008.
Fung, I., John, J., Lerner, J., Matthews, E., Prather, M., Steele, L., and
Fraser, P.: 3-Dimensional Model Synthesis of the Global Methane Cycle,
J. Geophys. Res.-Atmos., 96, 13033–13065,
https://doi.org/10.1029/91JD01247, 1991.
Ganesan, A., Stell, A., Gedney, N., Comyn-Platt, E., Hayman, G., Rigby, M.,
Poulter, B., and Hornibrook, E.: Spatially Resolved Isotopic Source
Signatures of Wetland Methane Emissions, Geophys. Res. Lett., 45,
3737–3745, 2018.
Gelaro, R., McCarty, W., Suarez, M., Todling, R., Molod, A., Takacs, L.,
Randles, C., Darmenov, A., Bosilovich, M., Reichle, R., Wargan, K., Coy, L.,
Cullather, R., Draper, C., Akella, S., Buchard, V., Conaty, A., da Silva,
A., Gu, W., Kim, G., Koster, R., Lucchesi, R., Merkova, D., Nielsen, J.,
Partyka, G., Pawson, S., Putman, W., Rienecker, M., Schubert, S.,
Sienkiewicz, M., and Zhao, B.: The Modern-Era Retrospective Analysis for
Research and Applications, Version 2 (MERRA-2), J. Climate, 30,
5419–5454, https://doi.org/10.1175/JCLI-D-16-0758.1, 2017.
Ghosh, A., Patra, P. K., Ishijima, K., Umezawa, T., Ito, A., Etheridge, D. M., Sugawara, S., Kawamura, K., Miller, J. B., Dlugokencky, E. J., Krummel, P. B., Fraser, P. J., Steele, L. P., Langenfelds, R. L., Trudinger, C. M., White, J. W. C., Vaughn, B., Saeki, T., Aoki, S., and Nakazawa, T.: Variations in global methane sources and sinks during 1910–2010, Atmos. Chem. Phys., 15, 2595–2612, https://doi.org/10.5194/acp-15-2595-2015, 2015.
Global Monitoring Laboratory: GML Data Finder, available at: https://www.esrl.noaa.gov/gmd/dv/data/, last access: 13 July 2020.
Granier, C., Bessagnet, B., Bond, T., D'Angiola, A., van der Gon, H. D.,
Frost, G. J., Heil, A., Kaiser, J. W., Kinne, S., Klimont, Z., Kloster, S.,
Lamarque, J. F., Liousse, C., Masui, T., Meleux, F., Mieville, A., Ohara,
T., Raut, J. C., Riahi, K., Schultz, M. G., Smith, S. J., Thompson, A., van
Aardenne, J., van der Werf, G. R., and van Vuuren, D. P.: Evolution of
anthropogenic and biomass burning emissions of air pollutants at global and
regional scales during the 1980-2010 period, Climatic Change, 109, 163–190,
https://doi.org/10.1007/s10584-011-0154-1, 2011.
Gromov, S., Brenninkmeijer, C. A. M., and Jöckel, P.: A very limited role of tropospheric chlorine as a sink of the greenhouse gas methane, Atmos. Chem. Phys., 18, 9831–9843, https://doi.org/10.5194/acp-18-9831-2018, 2018.
Hausmann, P., Sussmann, R., and Smale, D.: Contribution of oil and natural gas production to renewed increase in atmospheric methane (2007–2014): top–down estimate from ethane and methane column observations, Atmos. Chem. Phys., 16, 3227–3244, https://doi.org/10.5194/acp-16-3227-2016, 2016.
Hopcroft, P. O., Valdes, P. J., and Kaplan, J. O.: Bayesian Analysis of the
Glacial-Interglacial Methane Increase Constrained by Stable Isotopes and
Earth System Modeling, Geophys. Res. Lett., 45, 3653–3663,
https://doi.org/10.1002/2018GL077382, 2018.
Hossaini, R., Chipperfield, M. P., Saiz-Lopez, A., Fernandez, R., Monks, S.,
Feng, W., Brauer, P., and von Glasow, R.: A global model of tropospheric
chlorine chemistry: Organic versus inorganic sources and impact on methane
oxidation, J. Geophys. Res.-Atmos., 121,
14271–14297, https://doi.org/10.1002/2016JD025756, 2016.
Houweling, S., Kaminski, T., Dentener, F., Lelieveld, J., and Heimann, M.:
Inverse modeling of methane sources and sinks using the adjoint of a global
transport model, J. Geophys. Res.-Atmos., 104,
26137–26160, https://doi.org/10.1029/1999JD900428, 1999.
Houweling, S., Dentener, F., and Lelieveld, J.: Simulation of preindustrial
atmospheric methane to constrain the global source strength of natural
wetlands, J. Geophys. Res.-Atmos., 105, 17243–17255,
https://doi.org/10.1029/2000JD900193, 2000.
Houweling, S., Van der Werf, G., Goldewijk, K. K., Röckmann, T., and
Aben, I.: Early anthropogenic CH4 emissions and the variation of CH4 and
13CH4 over the last millennium, Global Biogeochem. Cy., 22, GB1002, https://doi.org/10.1029/2007GB002961, 2008.
Hu, L., Keller, C. A., Long, M. S., Sherwen, T., Auer, B., Da Silva, A., Nielsen, J. E., Pawson, S., Thompson, M. A., Trayanov, A. L., Travis, K. R., Grange, S. K., Evans, M. J., and Jacob, D. J.: Global simulation of tropospheric chemistry at 12.5 km resolution: performance and evaluation of the GEOS-Chem chemical module (v10-1) within the NASA GEOS Earth system model (GEOS-5 ESM), Geosci. Model Dev., 11, 4603–4620, https://doi.org/10.5194/gmd-11-4603-2018, 2018.
Ito, A. and Inatomi, M.: Use of a process-based model for assessing the methane budgets of global terrestrial ecosystems and evaluation of uncertainty, Biogeosciences, 9, 759–773, https://doi.org/10.5194/bg-9-759-2012, 2012.
Kai, F., Tyler, S., Randerson, J., and Blake, D.: Reduced methane growth
rate explained by decreased Northern Hemisphere microbial sources, Nature,
476, 194–197, https://doi.org/10.1038/nature10259, 2011.
Kirschke, S., Bousquet, P., Ciais, P., Saunois, M., Canadell, J. G.,
Dlugokencky, E. J., Bergamaschi, P., Bergmann, D., Blake, D. R., Bruhwiler,
L., Cameron-Smith, P., Castaldi, S., Chevallier, F., Feng, L., Fraser, A.,
Heimann, M., Hodson, E. L., Houweling, S., Josse, B., Fraser, P. J.,
Krummel, P. B., Lamarque, J.-F., Langenfelds, R. L., Le Quere, C., Naik, V.,
O'Doherty, S., Palmer, P. I., Pison, I., Plummer, D., Poulter, B., Prinn, R.
G., Rigby, M., Ringeval, B., Santini, M., Schmidt, M., Shindell, D. T.,
Simpson, I. J., Spahni, R., Steele, L. P., Strode, S. A., Sudo, K., Szopa,
S., van der Werf, G. R., Voulgarakis, A., van Weele, M., Weiss, R. F.,
Williams, J. E., and Zeng, G.: Three decades of global methane sources and
sinks, Nat. Geosci., 6, 813–823, https://doi.org/10.1038/NGEO1955, 2013.
Lassey, K. R., Etheridge, D. M., Lowe, D. C., Smith, A. M., and Ferretti, D. F.: Centennial evolution of the atmospheric methane budget: what do the carbon isotopes tell us?, Atmos. Chem. Phys., 7, 2119–2139, https://doi.org/10.5194/acp-7-2119-2007, 2007.
Long, M. S., Yantosca, R., Nielsen, J. E., Keller, C. A., da Silva, A., Sulprizio, M. P., Pawson, S., and Jacob, D. J.: Development of a grid-independent GEOS-Chem chemical transport model (v9-02) as an atmospheric chemistry module for Earth system models, Geosci. Model Dev., 8, 595–602, https://doi.org/10.5194/gmd-8-595-2015, 2015.
McNorton, J., Chipperfield, M. P., Gloor, M., Wilson, C., Feng, W., Hayman, G. D., Rigby, M., Krummel, P. B., O'Doherty, S., Prinn, R. G., Weiss, R. F., Young, D., Dlugokencky, E., and Montzka, S. A.: Role of OH variability in the stalling of the global atmospheric CH4 growth rate from 1999 to 2006, Atmos. Chem. Phys., 16, 7943–7956, https://doi.org/10.5194/acp-16-7943-2016, 2016.
Mikaloff Fletcher, S. E., Tans, P. P., Bruhwiler, L. M., Miller, J. B., and
Heimann, M.: CH4 sources estimated from atmospheric observations of CH4 and
its 13C∕12C isotopic ratios: 2. Inverse modeling of CH4 fluxes from
geographical regions, Global Biogeochem. Cy., 18, GB4005,
https://doi.org/10.1029/2004GB002224, 2004a.
Mikaloff Fletcher, S. E., Tans, P. P., Bruhwiler, L. M., Miller, J. B., and
Heimann, M.: CH4 sources estimated from atmospheric observations of CH4 and
its 13C∕12C isotopic ratios: 1. Inverse modeling of source processes, Global
Biogeochem. Cy., 18, GB4004, https://doi.org/10.1029/2004GB002223, 2004b.
Molod, A., Takacs, L., Suarez, M., and Bacmeister, J.: Development of the GEOS-5 atmospheric general circulation model: evolution from MERRA to MERRA2, Geosci. Model Dev., 8, 1339–1356, https://doi.org/10.5194/gmd-8-1339-2015, 2015.
Monteil, G., Houweling, S., Dlugockenky, E. J., Maenhout, G., Vaughn, B. H., White, J. W. C., and Rockmann, T.: Interpreting methane variations in the past two decades using measurements of CH4 mixing ratio and isotopic composition, Atmos. Chem. Phys., 11, 9141–9153, https://doi.org/10.5194/acp-11-9141-2011, 2011.
Naik, V., Voulgarakis, A., Fiore, A. M., Horowitz, L. W., Lamarque, J.-F., Lin, M., Prather, M. J., Young, P. J., Bergmann, D., Cameron-Smith, P. J., Cionni, I., Collins, W. J., Dalsøren, S. B., Doherty, R., Eyring, V., Faluvegi, G., Folberth, G. A., Josse, B., Lee, Y. H., MacKenzie, I. A., Nagashima, T., van Noije, T. P. C., Plummer, D. A., Righi, M., Rumbold, S. T., Skeie, R., Shindell, D. T., Stevenson, D. S., Strode, S., Sudo, K., Szopa, S., and Zeng, G.: Preindustrial to present-day changes in tropospheric hydroxyl radical and methane lifetime from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP), Atmos. Chem. Phys., 13, 5277–5298, https://doi.org/10.5194/acp-13-5277-2013, 2013.
Nielsen, J., Pawson, S., Molod, A., Auer, B., da Silva, A., Douglass, A.,
Duncan, B., Liang, Q., Manyin, M., Oman, L., Putman, W., Strahan, S., and
Wargan, K.: Chemical Mechanisms and Their Applications in the Goddard Earth
Observing System (GEOS) Earth System Model, J. Adv. Model.
Earth Sy., 9, 3019–3044, https://doi.org/10.1002/2017MS001011, 2017.
Nisbet, E., Dlugokencky, E., Manning, M., Lowry, D., Fisher, R., France, J.,
Michel, S., Miller, J., White, J., and Vaughn, B.: Rising atmospheric
methane: 2007–2014 growth and isotopic shift, Global Biogeochem. Cy.,
30, 1356–1370, 2016.
Nisbet, E., Manning, M., Dlugokencky, E., Fisher, R., Lowry, D., Michel, S.,
Myhre, C., Platt, M., Allen, G., Bousquet, P., Brownlow, R., Cain, M.,
France, J., Hermansen, O., Hossaini, R., Jones, A., Levin, I., Manning, A.,
Myhre, G., Pyle, J., Vaughn, B., Warwick, N., and White, J.: Very Strong.
Atmospheric Methane Growth in the 4 Years 2014–2017: Implications for the
paris Agreement, Global Biogeochem. Cy., 33, 318–342,
https://doi.org/10.1029/2018GB006009, 2019.
Orbe, C., Oman, L., Strahan, S., Waugh, D., Pawson, S., Takacs, L., and
Molod, A.: Large-Scale Atmospheric Transport in GEOS Replay Simulations,
J. Adv. Model. Earth Sy., 9, 2545–2560,
https://doi.org/10.1002/2017MS001053, 2017.
Patra, P. K., Houweling, S., Krol, M., Bousquet, P., Belikov, D., Bergmann, D., Bian, H., Cameron-Smith, P., Chipperfield, M. P., Corbin, K., Fortems-Cheiney, A., Fraser, A., Gloor, E., Hess, P., Ito, A., Kawa, S. R., Law, R. M., Loh, Z., Maksyutov, S., Meng, L., Palmer, P. I., Prinn, R. G., Rigby, M., Saito, R., and Wilson, C.: TransCom model simulations of CH4 and related species: linking transport, surface flux and chemical loss with CH4 variability in the troposphere and lower stratosphere, Atmos. Chem. Phys., 11, 12813–12837, https://doi.org/10.5194/acp-11-12813-2011, 2011.
Platt, U., Allan, W., and Lowe, D.: Hemispheric average Cl atom concentration from 13C∕12C ratios in atmospheric methane, Atmos. Chem. Phys., 4, 2393–2399, https://doi.org/10.5194/acp-4-2393-2004, 2004.
Quay, P., King, S., Stutsman, J., Wilbur, D., Steele, L., Fung, I., Gammon,
R., Brown, T., Farwell, G., Grootes, P., and Schmidt, F.: Carbon Isotopic
Composition of Atmospheric CH4: Fossil and Biomass Burning Source Strenghts,
Global Biogeochem. Cy., 5, 25–47, https://doi.org/10.1029/91GB00003, 1991.
Rice, A. L., Butenhoff, C. L., Teama, D. G., Röger, F. H., Khalil, M. A.
K., and Rasmussen, R. A.: Atmospheric methane isotopic record favors fossil
sources flat in 1980s and 1990s with recent increase, P.
Natl. Acad. Sci. USA, 113, 10791–10796, 2016.
Rigby, M., Prinn, R. G., Fraser, P. J., Simmonds, P. G., Langenfelds, R. L.,
Huang, J., Cunnold, D. M., Steele, L. P., Krummel, P. B., Weiss, R. F.,
O'Doherty, S., Salameh, P. K., Wang, H. J., Harth, C. M., Mühle, J., and
Porter, L. W.: Renewed growth of atmospheric methane, Geophys. Res.
Lett., 35, L22805, https://doi.org/10.1029/2008GL036037, 2008.
Rigby, M., Montzka, S. A., Prinn, R. G., White, J. W., Young, D., O'Doherty,
S., Lunt, M. F., Ganesan, A. L., Manning, A. J., and Simmonds, P. G.: Role
of atmospheric oxidation in recent methane growth, P.
Natl. Acad. Sci. USA, 114, 5373–5377, 2017.
Rotman, D., Tannahill, J., Kinnison, D., Connell, P., Bergmann, D., Proctor,
D., Rodriguez, J., Lin, S., Rood, R., Prather, M., Rasch, P., Considine, D.,
Ramaroson, R., and Kawa, S.: Global Modeling Initiative assessment model:
Model description, integration, and testing of the transport shell, J. Geophys. Res.-Atmos., 106, 1669–1691, https://doi.org/10.1029/2000JD900463,
2001.
Saueressig, G., Bergamaschi, P., Crowley, J., Fischer, H., and Harris, G.:
Carbon Kinetic Isotope Effect in the Reaction of CH4 with Cl Atoms,
Geophys. Res. Lett., 22, 1225–1228, https://doi.org/10.1029/95GL00881, 1995.
Saueressig, G., Crowley, J. N., Bergamaschi, P., Brühl, C.,
Brenninkmeijer, C. A. M., and Fischer, H.: Carbon 13 and D kinetic isotope
effects in the reactions of CH4 with O(1D) and OH: New laboratory
measurements and their implications for the isotopic composition of
stratospheric methane, J. Geophys. Res.-Atmos., 106,
23127–23138, https://doi.org/10.1029/2000JD000120, 2001.
Saunois, M., Bousquet, P., Poulter, B., Peregon, A., Ciais, P., Canadell, J. G., Dlugokencky, E. J., Etiope, G., Bastviken, D., Houweling, S., Janssens-Maenhout, G., Tubiello, F. N., Castaldi, S., Jackson, R. B., Alexe, M., Arora, V. K., Beerling, D. J., Bergamaschi, P., Blake, D. R., Brailsford, G., Bruhwiler, L., Crevoisier, C., Crill, P., Covey, K., Frankenberg, C., Gedney, N., Höglund-Isaksson, L., Ishizawa, M., Ito, A., Joos, F., Kim, H.-S., Kleinen, T., Krummel, P., Lamarque, J.-F., Langenfelds, R., Locatelli, R., Machida, T., Maksyutov, S., Melton, J. R., Morino, I., Naik, V., O'Doherty, S., Parmentier, F.-J. W., Patra, P. K., Peng, C., Peng, S., Peters, G. P., Pison, I., Prinn, R., Ramonet, M., Riley, W. J., Saito, M., Santini, M., Schroeder, R., Simpson, I. J., Spahni, R., Takizawa, A., Thornton, B. F., Tian, H., Tohjima, Y., Viovy, N., Voulgarakis, A., Weiss, R., Wilton, D. J., Wiltshire, A., Worthy, D., Wunch, D., Xu, X., Yoshida, Y., Zhang, B., Zhang, Z., and Zhu, Q.: Variability and quasi-decadal changes in the methane budget over the period 2000–2012, Atmos. Chem. Phys., 17, 11135–11161, https://doi.org/10.5194/acp-17-11135-2017, 2017.
Schaefer, H., Fletcher, S. E. M., Veidt, C., Lassey, K. R., Brailsford, G.
W., Bromley, T. M., Dlugokencky, E. J., Michel, S. E., Miller, J. B., Levin,
I., Lowe, D. C., Martin, R. J., Vaughn, B. H., and White, J. W. C.: A
21st-century shift from fossil-fuel to biogenic methane emissions indicated
by 13CH4, Science, 352, 80–84, https://doi.org/10.1126/science.aad2705, 2016.
Schwietzke, S., Sherwood, O., Ruhwiler, L., Miller, J., Etiope, G.,
Dlugokencky, E., Michel, S., Arling, V., Vaughn, B., White, J., and Tans,
P.: Upward revision of global fossil fuel methane emissions based on isotope
database, Nature, 538, 88–91, https://doi.org/10.1038/nature19797, 2016.
Sherwen, T., Schmidt, J. A., Evans, M. J., Carpenter, L. J., Großmann, K., Eastham, S. D., Jacob, D. J., Dix, B., Koenig, T. K., Sinreich, R., Ortega, I., Volkamer, R., Saiz-Lopez, A., Prados-Roman, C., Mahajan, A. S., and Ordóñez, C.: Global impacts of tropospheric halogens (Cl, Br, I) on oxidants and composition in GEOS-Chem, Atmos. Chem. Phys., 16, 12239–12271, https://doi.org/10.5194/acp-16-12239-2016, 2016.
Sherwood, O. A., Schwietzke, S., Arling, V. A., and Etiope, G.: Global Inventory of Gas Geochemistry Data from Fossil Fuel, Microbial and Burning Sources, version 2017, Earth Syst. Sci. Data, 9, 639–656, https://doi.org/10.5194/essd-9-639-2017, 2017.
Spivakovsky, C. M., Logan, J. A., Montzka, S. A., Balkanski, Y. J.,
Foreman-Fowler, M., Jones, D. B. A., Horowitz, L. W., Fusco, A. C.,
Brenninkmeijer, C. A. M., Prather, M. J., Wofsy, S. C., and McElroy, M. B.:
Three-dimensional climatological distribution of tropospheric OH: Update and
evaluation, J. Geophys. Res.-Atmos., 105, 8931–8980,
https://doi.org/10.1029/1999jd901006, 2000.
Strahan, S. E., Duncan, B. N., and Hoor, P.: Observationally derived transport diagnostics for the lowermost stratosphere and their application to the GMI chemistry and transport model, Atmos. Chem. Phys., 7, 2435–2445, https://doi.org/10.5194/acp-7-2435-2007, 2007.
Strahan, S. E., Douglass, A. R., and Newman, P. A.: The contributions of
chemistry and transport to low arctic ozone in March 2011 derived from Aura
MLS observations, J. Geophys. Res.-Atmos., 118,
1563–1576, 2013.
Strode, S. A., Duncan, B. N., Yegorova, E. A., Kouatchou, J., Ziemke, J. R., and Douglass, A. R.: Implications of carbon monoxide bias for methane lifetime and atmospheric composition in chemistry climate models, Atmos. Chem. Phys., 15, 11789–11805, https://doi.org/10.5194/acp-15-11789-2015, 2015.
Tans, P.: A note on isotopic ratios and the global atmospheric methane
budget, Global Biogeochem. Cy., 11, 77–81, https://doi.org/10.1029/96GB03940, 1997.
Thompson, R., Nisbet, E., Pisso, I., Stohl, A., Blake, D., Dlugokencky, E.,
Helmig, D., and White, J.: Variability in Atmospheric Methane From Fossil
Fuel and Microbial Sources Over the Last Three Decades, Geophys. Res.
Lett., 45, 11499–11508, https://doi.org/10.1029/2018GL078127, 2018.
Thompson, R. L., Stohl, A., Zhou, L. X., Dlugokencky, E., Fukuyama, Y.,
Tohjima, Y., Kim, S. Y., Lee, H., Nisbet, E. G., and Fisher, R. E.: Methane
emissions in East Asia for 2000–2011 estimated using an atmospheric
Bayesian inversion, J. Geophys. Res.-Atmos., 120,
4352–4369, 2015.
Turner, A., Jacob, D., Benmergui, J., Wofsy, S., Maasakkers, J., Butz, A.,
Hasekamp, O., and Biraud, S.: A large increase in US methane emissions over
the past decade inferred from satellite data and surface observations,
Geophys. Res. Lett., 43, 2218–2224, https://doi.org/10.1002/2016GL067987, 2016.
Turner, A. J., Frankenberg, C., Wennberg, P. O., and Jacob, D. J.: Ambiguity
in the causes for decadal trends in atmospheric methane and hydroxyl,
P. Natl. Acad. Sci. USA, 114, 5367–5372, 2017.
Tyler, S. C., Crill, P. M., and Brailsford, G. W.: 13C12C
Fractionation of methane during oxidation in a temperate forested soil,
Geochim. Cosmochim. Ac., 58, 1625–1633, https://doi.org/10.1016/0016-7037(94)90564-9,
1994.
Wang, J. S., McElroy, M. B., Spivakovsky, C. M., and Jones, D. B. A.: On the
contribution of anthropogenic Cl to the increase in δ13C of
atmospheric methane, Global Biogeochem. Cy., 16, 1047, https://doi.org/10.1029/2001GB001572, 2002.
Wang, X., Jacob, D. J., Eastham, S. D., Sulprizio, M. P., Zhu, L., Chen, Q., Alexander, B., Sherwen, T., Evans, M. J., Lee, B. H., Haskins, J. D., Lopez-Hilfiker, F. D., Thornton, J. A., Huey, G. L., and Liao, H.: The role of chlorine in global tropospheric chemistry, Atmos. Chem. Phys., 19, 3981–4003, https://doi.org/10.5194/acp-19-3981-2019, 2019.
Waugh, D., Crotwell, A., Dlugokencky, E., Dutton, G., Elkins, J., Hall, B.,
Hintsa, E., Hurst, D., Montzka, S., Mondeel, D., Moore, F., Nance, J., Ray,
E., Steenrod, S., Strahan, S., and Sweeney, C.: Tropospheric SF6: Age of air
from the Northern Hemisphere midlatitude surface, J. Geophys.
Res.-Atmos., 118, 11429–11441, https://doi.org/10.1002/jgrd.50848, 2013.
White, J. W. C., Vaughn, B. H., and Michel, S. E.: University of Colorado,
Institute of Arctic and Alpine Research (INSTAAR), Stable Isotopic
Composition of Atmospheric Methane (13C) from the NOAA ESRL Carbon Cycle
Cooperative Global Air Sampling Network, 1998–2017, Version: 2018-09-24, available at:
ftp://aftp.cmdl.noaa.gov/data/trace_gases/ch4c13/flask/ (last access: 30 January 2019), 2018.
Worden, J. R., Bloom, A. A., Pandey, S., Jiang, Z., Worden, H. M., Walker,
T. W., Houweling, S., and Röckmann, T.: Reduced biomass burning
emissions reconcile conflicting estimates of the post-2006 atmospheric
methane budget, Nat. Commun., 8, 2227, https://doi.org/10.1038/s41467-017-02246-0, 2017.
Zhang, Q.-L. and Li, W.-J.: A Calibrated Measurement of the Atomic Weight of
Carbon, Chinese Sci. Bull., 35, 290–296,
1990.
Short summary
The 13C : 12C isotopic ratio in methane (CH4) provides information about CH4 sources, but loss of CH4 by reaction with OH and chlorine (Cl) also affects this ratio. Tropospheric Cl provides a small and uncertain sink for CH4 but has a large effect on its isotopic ratio. We use the GEOS model with several different Cl fields to test the sensitivity of methane's isotopic composition to tropospheric Cl. Cl affects the global mean, hemispheric gradient, and seasonal cycle of the isotopic ratio.
The 13C : 12C isotopic ratio in methane (CH4) provides information about CH4 sources, but loss...
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