Articles | Volume 22, issue 4
https://doi.org/10.5194/acp-22-2871-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-22-2871-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
03 Mar 2022
Research article |
| 03 Mar 2022
| 03 Mar 2022
Stable carbon isotopic composition of biomass burning emissions – implications for estimating the contribution of C3 and C4 plants
Department of Earth Sciences, Faculty of Science, Vrije Universiteit Amsterdam, Amsterdam, the Netherlands
Ulrike Dusek
Centre for Isotope Research (CIO), Energy and Sustainability Research Institute Groningen (ESRIG), Rijksuniversiteit Groningen, Groningen, the Netherlands
Maria Elena Popa
Institute for Marine and Atmospheric research Utrecht, Utrecht University, Utrecht, the Netherlands
Centre for Isotope Research (CIO), Energy and Sustainability Research Institute Groningen (ESRIG), Rijksuniversiteit Groningen, Groningen, the Netherlands
Anupam Shaikat
Centre for Isotope Research (CIO), Energy and Sustainability Research Institute Groningen (ESRIG), Rijksuniversiteit Groningen, Groningen, the Netherlands
Chenxi Qiu
Institute for Marine and Atmospheric research Utrecht, Utrecht University, Utrecht, the Netherlands
IEK-7, Forschungszentrum Jülich GmbH, Jülich, Germany
Patrik Winiger
Department of Earth Sciences, Faculty of Science, Vrije Universiteit Amsterdam, Amsterdam, the Netherlands
Health and Environmental Department, Federal Institute of Technology (ETH) Zurich, Zurich, Switzerland
Carina van der Veen
Institute for Marine and Atmospheric research Utrecht, Utrecht University, Utrecht, the Netherlands
Thomas Callum Eames
Department of Earth Sciences, Faculty of Science, Vrije Universiteit Amsterdam, Amsterdam, the Netherlands
Natasha Ribeiro
Faculty of Agronomy and Forest Engineering, Eduardo Mondlane University, Maputo, Mozambique
Guido R. van der Werf
Department of Earth Sciences, Faculty of Science, Vrije Universiteit Amsterdam, Amsterdam, the Netherlands
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Leonard Kirago, Örjan Gustafsson, Samuel Mwaniki Gaita, Sophie L. Haslett, Michael J. Gatari, Maria Elena Popa, Thomas Röckmann, Christoph Zellweger, Martin Steinbacher, Jörg Klausen, Christian Félix, David Njiru, and August Andersson
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Roland Vernooij, Tom Eames, Jeremy Russell-Smith, Cameron Yates, Robin Beatty, Jay Evans, Andrew Edwards, Natasha Ribeiro, Martin Wooster, Tercia Strydom, Marcos Vinicius Giongo, Marco Assis Borges, Máximo Menezes Costa, Ana Carolina Sena Barradas, Dave van Wees, and Guido R. Van der Werf
Earth Syst. Dynam., 14, 1039–1064, https://doi.org/10.5194/esd-14-1039-2023, https://doi.org/10.5194/esd-14-1039-2023, 2023
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Marc von Hobe, Domenico Taraborrelli, Sascha Alber, Birger Bohn, Hans-Peter Dorn, Hendrik Fuchs, Yun Li, Chenxi Qiu, Franz Rohrer, Roberto Sommariva, Fred Stroh, Zhaofeng Tan, Sergej Wedel, and Anna Novelli
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Atmos. Chem. Phys., 23, 10399–10412, https://doi.org/10.5194/acp-23-10399-2023, https://doi.org/10.5194/acp-23-10399-2023, 2023
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Farhan R. Nursanto, Roy Meinen, Rupert Holzinger, Maarten C. Krol, Xinya Liu, Ulrike Dusek, Bas Henzing, and Juliane L. Fry
Atmos. Chem. Phys., 23, 10015–10034, https://doi.org/10.5194/acp-23-10015-2023, https://doi.org/10.5194/acp-23-10015-2023, 2023
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Andreas Forstmaier, Jia Chen, Florian Dietrich, Juan Bettinelli, Hossein Maazallahi, Carsten Schneider, Dominik Winkler, Xinxu Zhao, Taylor Jones, Carina van der Veen, Norman Wildmann, Moritz Makowski, Aydin Uzun, Friedrich Klappenbach, Hugo Denier van der Gon, Stefan Schwietzke, and Thomas Röckmann
Atmos. Chem. Phys., 23, 6897–6922, https://doi.org/10.5194/acp-23-6897-2023, https://doi.org/10.5194/acp-23-6897-2023, 2023
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Ana Maria Roxana Petrescu, Chunjing Qiu, Matthew J. McGrath, Philippe Peylin, Glen P. Peters, Philippe Ciais, Rona L. Thompson, Aki Tsuruta, Dominik Brunner, Matthias Kuhnert, Bradley Matthews, Paul I. Palmer, Oksana Tarasova, Pierre Regnier, Ronny Lauerwald, David Bastviken, Lena Höglund-Isaksson, Wilfried Winiwarter, Giuseppe Etiope, Tuula Aalto, Gianpaolo Balsamo, Vladislav Bastrikov, Antoine Berchet, Patrick Brockmann, Giancarlo Ciotoli, Giulia Conchedda, Monica Crippa, Frank Dentener, Christine D. Groot Zwaaftink, Diego Guizzardi, Dirk Günther, Jean-Matthieu Haussaire, Sander Houweling, Greet Janssens-Maenhout, Massaer Kouyate, Adrian Leip, Antti Leppänen, Emanuele Lugato, Manon Maisonnier, Alistair J. Manning, Tiina Markkanen, Joe McNorton, Marilena Muntean, Gabriel D. Oreggioni, Prabir K. Patra, Lucia Perugini, Isabelle Pison, Maarit T. Raivonen, Marielle Saunois, Arjo J. Segers, Pete Smith, Efisio Solazzo, Hanqin Tian, Francesco N. Tubiello, Timo Vesala, Guido R. van der Werf, Chris Wilson, and Sönke Zaehle
Earth Syst. Sci. Data, 15, 1197–1268, https://doi.org/10.5194/essd-15-1197-2023, https://doi.org/10.5194/essd-15-1197-2023, 2023
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This study updates the state-of-the-art scientific overview of CH4 and N2O emissions in the EU27 and UK in Petrescu et al. (2021a). Yearly updates are needed to improve the different respective approaches and to inform on the development of formal verification systems. It integrates the most recent emission inventories, process-based model and regional/global inversions, comparing them with UNFCCC national GHG inventories, in support to policy to facilitate real-time verification procedures.
Bryce F. J. Kelly, Xinyi Lu, Stephen J. Harris, Bruno G. Neininger, Jorg M. Hacker, Stefan Schwietzke, Rebecca E. Fisher, James L. France, Euan G. Nisbet, David Lowry, Carina van der Veen, Malika Menoud, and Thomas Röckmann
Atmos. Chem. Phys., 22, 15527–15558, https://doi.org/10.5194/acp-22-15527-2022, https://doi.org/10.5194/acp-22-15527-2022, 2022
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This study explores using the composition of methane of in-flight atmospheric air samples for greenhouse gas inventory verification. The air samples were collected above one of the largest coal seam gas production regions in the world. Adjacent to these gas fields are coal mines, Australia's largest cattle feedlot, and over 1 million grazing cattle. The results are also used to identify methane mitigation opportunities.
Dave van Wees, Guido R. van der Werf, James T. Randerson, Brendan M. Rogers, Yang Chen, Sander Veraverbeke, Louis Giglio, and Douglas C. Morton
Geosci. Model Dev., 15, 8411–8437, https://doi.org/10.5194/gmd-15-8411-2022, https://doi.org/10.5194/gmd-15-8411-2022, 2022
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We present a global fire emission model based on the GFED model framework with a spatial resolution of 500 m. The higher resolution allowed for a more detailed representation of spatial heterogeneity in fuels and emissions. Specific modules were developed to model, for example, emissions from fire-related forest loss and belowground burning. Results from the 500 m model were compared to GFED4s, showing that global emissions were relatively similar but that spatial differences were substantial.
Pierre Friedlingstein, Michael O'Sullivan, Matthew W. Jones, Robbie M. Andrew, Luke Gregor, Judith Hauck, Corinne Le Quéré, Ingrid T. Luijkx, Are Olsen, Glen P. Peters, Wouter Peters, Julia Pongratz, Clemens Schwingshackl, Stephen Sitch, Josep G. Canadell, Philippe Ciais, Robert B. Jackson, Simone R. Alin, Ramdane Alkama, Almut Arneth, Vivek K. Arora, Nicholas R. Bates, Meike Becker, Nicolas Bellouin, Henry C. Bittig, Laurent Bopp, Frédéric Chevallier, Louise P. Chini, Margot Cronin, Wiley Evans, Stefanie Falk, Richard A. Feely, Thomas Gasser, Marion Gehlen, Thanos Gkritzalis, Lucas Gloege, Giacomo Grassi, Nicolas Gruber, Özgür Gürses, Ian Harris, Matthew Hefner, Richard A. Houghton, George C. Hurtt, Yosuke Iida, Tatiana Ilyina, Atul K. Jain, Annika Jersild, Koji Kadono, Etsushi Kato, Daniel Kennedy, Kees Klein Goldewijk, Jürgen Knauer, Jan Ivar Korsbakken, Peter Landschützer, Nathalie Lefèvre, Keith Lindsay, Junjie Liu, Zhu Liu, Gregg Marland, Nicolas Mayot, Matthew J. McGrath, Nicolas Metzl, Natalie M. Monacci, David R. Munro, Shin-Ichiro Nakaoka, Yosuke Niwa, Kevin O'Brien, Tsuneo Ono, Paul I. Palmer, Naiqing Pan, Denis Pierrot, Katie Pocock, Benjamin Poulter, Laure Resplandy, Eddy Robertson, Christian Rödenbeck, Carmen Rodriguez, Thais M. Rosan, Jörg Schwinger, Roland Séférian, Jamie D. Shutler, Ingunn Skjelvan, Tobias Steinhoff, Qing Sun, Adrienne J. Sutton, Colm Sweeney, Shintaro Takao, Toste Tanhua, Pieter P. Tans, Xiangjun Tian, Hanqin Tian, Bronte Tilbrook, Hiroyuki Tsujino, Francesco Tubiello, Guido R. van der Werf, Anthony P. Walker, Rik Wanninkhof, Chris Whitehead, Anna Willstrand Wranne, Rebecca Wright, Wenping Yuan, Chao Yue, Xu Yue, Sönke Zaehle, Jiye Zeng, and Bo Zheng
Earth Syst. Sci. Data, 14, 4811–4900, https://doi.org/10.5194/essd-14-4811-2022, https://doi.org/10.5194/essd-14-4811-2022, 2022
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The Global Carbon Budget 2022 describes the datasets and methodology used to quantify the anthropogenic emissions of carbon dioxide (CO2) and their partitioning among the atmosphere, the land ecosystems, and the ocean. These living datasets are updated every year to provide the highest transparency and traceability in the reporting of CO2, the key driver of climate change.
Malika Menoud, Carina van der Veen, Dave Lowry, Julianne M. Fernandez, Semra Bakkaloglu, James L. France, Rebecca E. Fisher, Hossein Maazallahi, Mila Stanisavljević, Jarosław Nęcki, Katarina Vinkovic, Patryk Łakomiec, Janne Rinne, Piotr Korbeń, Martina Schmidt, Sara Defratyka, Camille Yver-Kwok, Truls Andersen, Huilin Chen, and Thomas Röckmann
Earth Syst. Sci. Data, 14, 4365–4386, https://doi.org/10.5194/essd-14-4365-2022, https://doi.org/10.5194/essd-14-4365-2022, 2022
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Emission sources of methane (CH4) can be distinguished with measurements of CH4 stable isotopes. We present new measurements of isotope signatures of various CH4 sources in Europe, mainly anthropogenic, sampled from 2017 to 2020. The present database also contains the most recent update of the global signature dataset from the literature. The dataset improves CH4 source attribution and the understanding of the global CH4 budget.
Qirui Zhong, Nick Schutgens, Guido van der Werf, Twan van Noije, Kostas Tsigaridis, Susanne E. Bauer, Tero Mielonen, Alf Kirkevåg, Øyvind Seland, Harri Kokkola, Ramiro Checa-Garcia, David Neubauer, Zak Kipling, Hitoshi Matsui, Paul Ginoux, Toshihiko Takemura, Philippe Le Sager, Samuel Rémy, Huisheng Bian, Mian Chin, Kai Zhang, Jialei Zhu, Svetlana G. Tsyro, Gabriele Curci, Anna Protonotariou, Ben Johnson, Joyce E. Penner, Nicolas Bellouin, Ragnhild B. Skeie, and Gunnar Myhre
Atmos. Chem. Phys., 22, 11009–11032, https://doi.org/10.5194/acp-22-11009-2022, https://doi.org/10.5194/acp-22-11009-2022, 2022
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Aerosol optical depth (AOD) errors for biomass burning aerosol (BBA) are evaluated in 18 global models against satellite datasets. Notwithstanding biases in satellite products, they allow model evaluations. We observe large and diverse model biases due to errors in BBA. Further interpretations of AOD diversities suggest large biases exist in key processes for BBA which require better constraining. These results can contribute to further model improvement and development.
Roland Vernooij, Patrik Winiger, Martin Wooster, Tercia Strydom, Laurent Poulain, Ulrike Dusek, Mark Grosvenor, Gareth J. Roberts, Nick Schutgens, and Guido R. van der Werf
Atmos. Meas. Tech., 15, 4271–4294, https://doi.org/10.5194/amt-15-4271-2022, https://doi.org/10.5194/amt-15-4271-2022, 2022
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Landscape fires are a substantial emitter of greenhouse gases and aerosols. Previous studies have indicated savanna emission factors to be highly variable. Improving fire emission estimates, and understanding future climate- and human-induced changes in fire regimes, requires in situ measurements. We present a drone-based method that enables the collection of a large amount of high-quality emission factor measurements that do not have the biases of aircraft or surface measurements.
Pierre Friedlingstein, Matthew W. Jones, Michael O'Sullivan, Robbie M. Andrew, Dorothee C. E. Bakker, Judith Hauck, Corinne Le Quéré, Glen P. Peters, Wouter Peters, Julia Pongratz, Stephen Sitch, Josep G. Canadell, Philippe Ciais, Rob B. Jackson, Simone R. Alin, Peter Anthoni, Nicholas R. Bates, Meike Becker, Nicolas Bellouin, Laurent Bopp, Thi Tuyet Trang Chau, Frédéric Chevallier, Louise P. Chini, Margot Cronin, Kim I. Currie, Bertrand Decharme, Laique M. Djeutchouang, Xinyu Dou, Wiley Evans, Richard A. Feely, Liang Feng, Thomas Gasser, Dennis Gilfillan, Thanos Gkritzalis, Giacomo Grassi, Luke Gregor, Nicolas Gruber, Özgür Gürses, Ian Harris, Richard A. Houghton, George C. Hurtt, Yosuke Iida, Tatiana Ilyina, Ingrid T. Luijkx, Atul Jain, Steve D. Jones, Etsushi Kato, Daniel Kennedy, Kees Klein Goldewijk, Jürgen Knauer, Jan Ivar Korsbakken, Arne Körtzinger, Peter Landschützer, Siv K. Lauvset, Nathalie Lefèvre, Sebastian Lienert, Junjie Liu, Gregg Marland, Patrick C. McGuire, Joe R. Melton, David R. Munro, Julia E. M. S. Nabel, Shin-Ichiro Nakaoka, Yosuke Niwa, Tsuneo Ono, Denis Pierrot, Benjamin Poulter, Gregor Rehder, Laure Resplandy, Eddy Robertson, Christian Rödenbeck, Thais M. Rosan, Jörg Schwinger, Clemens Schwingshackl, Roland Séférian, Adrienne J. Sutton, Colm Sweeney, Toste Tanhua, Pieter P. Tans, Hanqin Tian, Bronte Tilbrook, Francesco Tubiello, Guido R. van der Werf, Nicolas Vuichard, Chisato Wada, Rik Wanninkhof, Andrew J. Watson, David Willis, Andrew J. Wiltshire, Wenping Yuan, Chao Yue, Xu Yue, Sönke Zaehle, and Jiye Zeng
Earth Syst. Sci. Data, 14, 1917–2005, https://doi.org/10.5194/essd-14-1917-2022, https://doi.org/10.5194/essd-14-1917-2022, 2022
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The Global Carbon Budget 2021 describes the data sets and methodology used to quantify the emissions of carbon dioxide and their partitioning among the atmosphere, land, and ocean. These living data are updated every year to provide the highest transparency and traceability in the reporting of CO2, the key driver of climate change.
Stephen M. Platt, Øystein Hov, Torunn Berg, Knut Breivik, Sabine Eckhardt, Konstantinos Eleftheriadis, Nikolaos Evangeliou, Markus Fiebig, Rebecca Fisher, Georg Hansen, Hans-Christen Hansson, Jost Heintzenberg, Ove Hermansen, Dominic Heslin-Rees, Kim Holmén, Stephen Hudson, Roland Kallenborn, Radovan Krejci, Terje Krognes, Steinar Larssen, David Lowry, Cathrine Lund Myhre, Chris Lunder, Euan Nisbet, Pernilla B. Nizzetto, Ki-Tae Park, Christina A. Pedersen, Katrine Aspmo Pfaffhuber, Thomas Röckmann, Norbert Schmidbauer, Sverre Solberg, Andreas Stohl, Johan Ström, Tove Svendby, Peter Tunved, Kjersti Tørnkvist, Carina van der Veen, Stergios Vratolis, Young Jun Yoon, Karl Espen Yttri, Paul Zieger, Wenche Aas, and Kjetil Tørseth
Atmos. Chem. Phys., 22, 3321–3369, https://doi.org/10.5194/acp-22-3321-2022, https://doi.org/10.5194/acp-22-3321-2022, 2022
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Here we detail the history of the Zeppelin Observatory, a unique global background site and one of only a few in the high Arctic. We present long-term time series of up to 30 years of atmospheric components and atmospheric transport phenomena. Many of these time series are important to our understanding of Arctic and global atmospheric composition change. Finally, we discuss the future of the Zeppelin Observatory and emerging areas of future research on the Arctic atmosphere.
Malika Menoud, Carina van der Veen, Jaroslaw Necki, Jakub Bartyzel, Barbara Szénási, Mila Stanisavljević, Isabelle Pison, Philippe Bousquet, and Thomas Röckmann
Atmos. Chem. Phys., 21, 13167–13185, https://doi.org/10.5194/acp-21-13167-2021, https://doi.org/10.5194/acp-21-13167-2021, 2021
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Using measurements of methane isotopes in ambient air and a 3D atmospheric transport model, in Krakow, Poland, we mainly detected fossil-fuel-related sources, coming from coal mining in Silesia and from the use of natural gas in the city. Emission inventories report large emissions from coal mine activity in Silesia, which is in agreement with our measurements. However, methane sources in the urban area of Krakow related to the use of fossil fuels might be underestimated in the inventories.
Corinna Kloss, Vicheith Tan, J. Brian Leen, Garrett L. Madsen, Aaron Gardner, Xu Du, Thomas Kulessa, Johannes Schillings, Herbert Schneider, Stefanie Schrade, Chenxi Qiu, and Marc von Hobe
Atmos. Meas. Tech., 14, 5271–5297, https://doi.org/10.5194/amt-14-5271-2021, https://doi.org/10.5194/amt-14-5271-2021, 2021
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We describe the innovative analyzer
AMICAfor airborne trace gas measurements by infrared spectroscopy. Its design makes it robust and allows for sensitive measurements. AMICA has been used on two different aircraft for measuring gases including carbonyl sulfide, carbon monoxide and ozone. With fairly simple adaptions, AMICA can measure many stable trace gases that absorb light in the infrared.
Xinyi Lu, Stephen J. Harris, Rebecca E. Fisher, James L. France, Euan G. Nisbet, David Lowry, Thomas Röckmann, Carina van der Veen, Malika Menoud, Stefan Schwietzke, and Bryce F. J. Kelly
Atmos. Chem. Phys., 21, 10527–10555, https://doi.org/10.5194/acp-21-10527-2021, https://doi.org/10.5194/acp-21-10527-2021, 2021
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Many coal seam gas (CSG) facilities in the Surat Basin, Australia, are adjacent to other sources of methane, including agricultural, urban, and natural seeps. This makes it challenging to estimate the amount of methane being emitted into the atmosphere from CSG facilities. This research demonstrates that measurements of the carbon and hydrogen stable isotopic composition of methane can distinguish between and apportion methane emissions from CSG facilities, cattle, and many other sources.
Wei Yuan, Ru-Jin Huang, Lu Yang, Ting Wang, Jing Duan, Jie Guo, Haiyan Ni, Yang Chen, Qi Chen, Yongjie Li, Ulrike Dusek, Colin O'Dowd, and Thorsten Hoffmann
Atmos. Chem. Phys., 21, 3685–3697, https://doi.org/10.5194/acp-21-3685-2021, https://doi.org/10.5194/acp-21-3685-2021, 2021
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We characterized the seasonal variations in nitrated aromatic compounds (NACs) in composition, sources, and their light absorption contribution to brown carbon (BrC) aerosol in Xi'an, Northwest China. Our results show that secondary formation and vehicular emission were dominant sources in summer (~80 %), and biomass burning and coal combustion were major sources in winter (~75 %), and they indicate that the composition and sources of NACs have a profound impact on the light absorption of BrC
Roland Vernooij, Marcos Giongo, Marco Assis Borges, Máximo Menezes Costa, Ana Carolina Sena Barradas, and Guido R. van der Werf
Biogeosciences, 18, 1375–1393, https://doi.org/10.5194/bg-18-1375-2021, https://doi.org/10.5194/bg-18-1375-2021, 2021
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We used drones to measure greenhouse gas emission factors from fires in the Brazilian Cerrado. We compared early-dry-season management fires and late-dry-season fires to determine if fire management can be a tool for abating emissions.
Although we found some evidence of increased CO and CH4 emission factors, the seasonal effect was smaller than that found in previous studies. For N2O, the third most important greenhouse gas, we found opposite trends in grass- and shrub-dominated areas.
Ivar R. van der Velde, Guido R. van der Werf, Sander Houweling, Henk J. Eskes, J. Pepijn Veefkind, Tobias Borsdorff, and Ilse Aben
Atmos. Chem. Phys., 21, 597–616, https://doi.org/10.5194/acp-21-597-2021, https://doi.org/10.5194/acp-21-597-2021, 2021
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This paper compares the relative atmospheric enhancements of CO and NO2 measured by the space-based instrument TROPOMI over different fire-prone ecosystems around the world. We find distinct spatial and temporal patterns in the ΔNO2 / ΔCO ratio that correspond to regional differences in combustion efficiency. This joint analysis provides a better understanding of regional-scale combustion characteristics and can help the fire modeling community to improve existing global emission inventories.
Haiyan Ni, Ru-Jin Huang, Max M. Cosijn, Lu Yang, Jie Guo, Junji Cao, and Ulrike Dusek
Atmos. Chem. Phys., 20, 16041–16053, https://doi.org/10.5194/acp-20-16041-2020, https://doi.org/10.5194/acp-20-16041-2020, 2020
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We investigated sources of carbonaceous aerosols in Beijing and Xi'an during severe winter haze. Elemental carbon (EC) was dominated by vehicle emissions in Xi’an and coal burning in Beijing. Organic carbon (OC) increment during haze days was driven by the increase in primary and secondary OC (SOC). SOC was more from fossil sources in Beijing than Xi’an, especially during haze days. In Xi’an, no strong day–night differences in EC or OC sources suggest a large accumulation of particles.
Pierre Friedlingstein, Michael O'Sullivan, Matthew W. Jones, Robbie M. Andrew, Judith Hauck, Are Olsen, Glen P. Peters, Wouter Peters, Julia Pongratz, Stephen Sitch, Corinne Le Quéré, Josep G. Canadell, Philippe Ciais, Robert B. Jackson, Simone Alin, Luiz E. O. C. Aragão, Almut Arneth, Vivek Arora, Nicholas R. Bates, Meike Becker, Alice Benoit-Cattin, Henry C. Bittig, Laurent Bopp, Selma Bultan, Naveen Chandra, Frédéric Chevallier, Louise P. Chini, Wiley Evans, Liesbeth Florentie, Piers M. Forster, Thomas Gasser, Marion Gehlen, Dennis Gilfillan, Thanos Gkritzalis, Luke Gregor, Nicolas Gruber, Ian Harris, Kerstin Hartung, Vanessa Haverd, Richard A. Houghton, Tatiana Ilyina, Atul K. Jain, Emilie Joetzjer, Koji Kadono, Etsushi Kato, Vassilis Kitidis, Jan Ivar Korsbakken, Peter Landschützer, Nathalie Lefèvre, Andrew Lenton, Sebastian Lienert, Zhu Liu, Danica Lombardozzi, Gregg Marland, Nicolas Metzl, David R. Munro, Julia E. M. S. Nabel, Shin-Ichiro Nakaoka, Yosuke Niwa, Kevin O'Brien, Tsuneo Ono, Paul I. Palmer, Denis Pierrot, Benjamin Poulter, Laure Resplandy, Eddy Robertson, Christian Rödenbeck, Jörg Schwinger, Roland Séférian, Ingunn Skjelvan, Adam J. P. Smith, Adrienne J. Sutton, Toste Tanhua, Pieter P. Tans, Hanqin Tian, Bronte Tilbrook, Guido van der Werf, Nicolas Vuichard, Anthony P. Walker, Rik Wanninkhof, Andrew J. Watson, David Willis, Andrew J. Wiltshire, Wenping Yuan, Xu Yue, and Sönke Zaehle
Earth Syst. Sci. Data, 12, 3269–3340, https://doi.org/10.5194/essd-12-3269-2020, https://doi.org/10.5194/essd-12-3269-2020, 2020
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The Global Carbon Budget 2020 describes the data sets and methodology used to quantify the emissions of carbon dioxide and their partitioning among the atmosphere, land, and ocean. These living data are updated every year to provide the highest transparency and traceability in the reporting of CO2, the key driver of climate change.
Joram J. D. Hooghiem, Maria Elena Popa, Thomas Röckmann, Jens-Uwe Grooß, Ines Tritscher, Rolf Müller, Rigel Kivi, and Huilin Chen
Atmos. Chem. Phys., 20, 13985–14003, https://doi.org/10.5194/acp-20-13985-2020, https://doi.org/10.5194/acp-20-13985-2020, 2020
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Wildfires release a large quantity of pollutants that can reach the stratosphere through pyro-convection events. In September 2017, a stratospheric plume was accidentally sampled during balloon soundings in northern Finland. The source of the plume was identified to be wildfire smoke based on in situ measurements of carbon monoxide (CO) and stable isotope analysis of CO. Furthermore, the age of the plume was estimated using backwards transport modelling to be ~24 d, with its origin in Canada.
Marielle Saunois, Ann R. Stavert, Ben Poulter, Philippe Bousquet, Josep G. Canadell, Robert B. Jackson, Peter A. Raymond, Edward J. Dlugokencky, Sander Houweling, Prabir K. Patra, Philippe Ciais, Vivek K. Arora, David Bastviken, Peter Bergamaschi, Donald R. Blake, Gordon Brailsford, Lori Bruhwiler, Kimberly M. Carlson, Mark Carrol, Simona Castaldi, Naveen Chandra, Cyril Crevoisier, Patrick M. Crill, Kristofer Covey, Charles L. Curry, Giuseppe Etiope, Christian Frankenberg, Nicola Gedney, Michaela I. Hegglin, Lena Höglund-Isaksson, Gustaf Hugelius, Misa Ishizawa, Akihiko Ito, Greet Janssens-Maenhout, Katherine M. Jensen, Fortunat Joos, Thomas Kleinen, Paul B. Krummel, Ray L. Langenfelds, Goulven G. Laruelle, Licheng Liu, Toshinobu Machida, Shamil Maksyutov, Kyle C. McDonald, Joe McNorton, Paul A. Miller, Joe R. Melton, Isamu Morino, Jurek Müller, Fabiola Murguia-Flores, Vaishali Naik, Yosuke Niwa, Sergio Noce, Simon O'Doherty, Robert J. Parker, Changhui Peng, Shushi Peng, Glen P. Peters, Catherine Prigent, Ronald Prinn, Michel Ramonet, Pierre Regnier, William J. Riley, Judith A. Rosentreter, Arjo Segers, Isobel J. Simpson, Hao Shi, Steven J. Smith, L. Paul Steele, Brett F. Thornton, Hanqin Tian, Yasunori Tohjima, Francesco N. Tubiello, Aki Tsuruta, Nicolas Viovy, Apostolos Voulgarakis, Thomas S. Weber, Michiel van Weele, Guido R. van der Werf, Ray F. Weiss, Doug Worthy, Debra Wunch, Yi Yin, Yukio Yoshida, Wenxin Zhang, Zhen Zhang, Yuanhong Zhao, Bo Zheng, Qing Zhu, Qiuan Zhu, and Qianlai Zhuang
Earth Syst. Sci. Data, 12, 1561–1623, https://doi.org/10.5194/essd-12-1561-2020, https://doi.org/10.5194/essd-12-1561-2020, 2020
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Understanding and quantifying the global methane (CH4) budget is important for assessing realistic pathways to mitigate climate change. We have established a consortium of multidisciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate new research aimed at improving and regularly updating the global methane budget. This is the second version of the review dedicated to the decadal methane budget, integrating results of top-down and bottom-up estimates.
Leyang Feng, Steven J. Smith, Caleb Braun, Monica Crippa, Matthew J. Gidden, Rachel Hoesly, Zbigniew Klimont, Margreet van Marle, Maarten van den Berg, and Guido R. van der Werf
Geosci. Model Dev., 13, 461–482, https://doi.org/10.5194/gmd-13-461-2020, https://doi.org/10.5194/gmd-13-461-2020, 2020
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We describe the methods used for generating gridded emission datasets produced for use by the modeling community, particularly for the Coupled Model Intercomparison Project Phase 6 (CMIP6). The development of three sets of gridded data (historical open burning, historical anthropogenic, and future scenarios) was coordinated to produce consistent data over 1750–2100. We discuss the methodologies used to produce these data along with limitations and potential for future work.
Haiyan Ni, Ru-Jin Huang, Junji Cao, Jie Guo, Haoyue Deng, and Ulrike Dusek
Atmos. Chem. Phys., 19, 15609–15628, https://doi.org/10.5194/acp-19-15609-2019, https://doi.org/10.5194/acp-19-15609-2019, 2019
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We present a 1-year source apportionment record of carbonaceous aerosols in Xi'an, China. Biomass burning strongly increases in winter, while seasonal changes of coal and liquid fossil fuel combustion are moderate. We find strong evidence for fossil secondary OC formation during the warm period that is further enhanced in stagnant, polluted conditions due to longer atmospheric residence times. At the same time we find that water-insoluble (primary) fossil is lost due to photochemical processing.
Pierre Friedlingstein, Matthew W. Jones, Michael O'Sullivan, Robbie M. Andrew, Judith Hauck, Glen P. Peters, Wouter Peters, Julia Pongratz, Stephen Sitch, Corinne Le Quéré, Dorothee C. E. Bakker, Josep G. Canadell, Philippe Ciais, Robert B. Jackson, Peter Anthoni, Leticia Barbero, Ana Bastos, Vladislav Bastrikov, Meike Becker, Laurent Bopp, Erik Buitenhuis, Naveen Chandra, Frédéric Chevallier, Louise P. Chini, Kim I. Currie, Richard A. Feely, Marion Gehlen, Dennis Gilfillan, Thanos Gkritzalis, Daniel S. Goll, Nicolas Gruber, Sören Gutekunst, Ian Harris, Vanessa Haverd, Richard A. Houghton, George Hurtt, Tatiana Ilyina, Atul K. Jain, Emilie Joetzjer, Jed O. Kaplan, Etsushi Kato, Kees Klein Goldewijk, Jan Ivar Korsbakken, Peter Landschützer, Siv K. Lauvset, Nathalie Lefèvre, Andrew Lenton, Sebastian Lienert, Danica Lombardozzi, Gregg Marland, Patrick C. McGuire, Joe R. Melton, Nicolas Metzl, David R. Munro, Julia E. M. S. Nabel, Shin-Ichiro Nakaoka, Craig Neill, Abdirahman M. Omar, Tsuneo Ono, Anna Peregon, Denis Pierrot, Benjamin Poulter, Gregor Rehder, Laure Resplandy, Eddy Robertson, Christian Rödenbeck, Roland Séférian, Jörg Schwinger, Naomi Smith, Pieter P. Tans, Hanqin Tian, Bronte Tilbrook, Francesco N. Tubiello, Guido R. van der Werf, Andrew J. Wiltshire, and Sönke Zaehle
Earth Syst. Sci. Data, 11, 1783–1838, https://doi.org/10.5194/essd-11-1783-2019, https://doi.org/10.5194/essd-11-1783-2019, 2019
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The Global Carbon Budget 2019 describes the data sets and methodology used to quantify the emissions of carbon dioxide and their partitioning among the atmosphere, land, and ocean. These living data are updated every year to provide the highest transparency and traceability in the reporting of CO2, the key driver of climate change.
Dave van Wees and Guido R. van der Werf
Geosci. Model Dev., 12, 4681–4703, https://doi.org/10.5194/gmd-12-4681-2019, https://doi.org/10.5194/gmd-12-4681-2019, 2019
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For this paper, a novel high spatial-resolution fire emission model based on the Global Fire Emissions Database (GFED) modelling framework was developed and compared to a coarser-resolution version of the same model. Our findings highlight the importance of fine spatial resolution when modelling global-scale fire emissions, especially considering the comparison of model pixels to individual field measurements and the model representation of heterogeneity in the landscape.
Fang Li, Maria Val Martin, Meinrat O. Andreae, Almut Arneth, Stijn Hantson, Johannes W. Kaiser, Gitta Lasslop, Chao Yue, Dominique Bachelet, Matthew Forrest, Erik Kluzek, Xiaohong Liu, Stephane Mangeon, Joe R. Melton, Daniel S. Ward, Anton Darmenov, Thomas Hickler, Charles Ichoku, Brian I. Magi, Stephen Sitch, Guido R. van der Werf, Christine Wiedinmyer, and Sam S. Rabin
Atmos. Chem. Phys., 19, 12545–12567, https://doi.org/10.5194/acp-19-12545-2019, https://doi.org/10.5194/acp-19-12545-2019, 2019
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Fire emissions are critical for atmospheric composition, climate, carbon cycle, and air quality. We provide the first global multi-model fire emission reconstructions for 1700–2012, including carbon and 33 species of trace gases and aerosols, based on the nine state-of-the-art global fire models that participated in FireMIP. We also provide information on the recent status and limitations of the model-based reconstructions and identify the main uncertainty sources in their long-term changes.
Haiyan Ni, Ru-Jin Huang, Junji Cao, Wenting Dai, Jiamao Zhou, Haoyue Deng, Anita Aerts-Bijma, Harro A. J. Meijer, and Ulrike Dusek
Atmos. Chem. Phys., 19, 10405–10422, https://doi.org/10.5194/acp-19-10405-2019, https://doi.org/10.5194/acp-19-10405-2019, 2019
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We apply radiocarbon source apportionment of more volatile organic carbon (mvOC) to winter aerosol samples from six Chinese cities. We find a consistently larger contribution of fossil sources to mvOC than to secondary or total organic carbon. Fossil mvOC concentrations are strongly correlated with primary fossil OC but not with secondary fossil OC. The variability in nonfossil mvOC seems to be related to both primary and secondary biomass burning sources.
Jing Duan, Ru-Jin Huang, Chunshui Lin, Wenting Dai, Meng Wang, Yifang Gu, Ying Wang, Haobin Zhong, Yan Zheng, Haiyan Ni, Uli Dusek, Yang Chen, Yongjie Li, Qi Chen, Douglas R. Worsnop, Colin D. O'Dowd, and Junji Cao
Atmos. Chem. Phys., 19, 10319–10334, https://doi.org/10.5194/acp-19-10319-2019, https://doi.org/10.5194/acp-19-10319-2019, 2019
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We present the seasonal distinction of secondary aerosol formation in urban Beijing. Both photochemical oxidation and aqueous-phase processing played important roles in SOA (secondary organic aerosol) formation during all three seasons; while for sulfate formation, gas-phase photochemical oxidation was the major pathway in late summer, aqueous-phase reactions were more responsible during early winter, and both processes had contributions during autumn.
Niels Andela, Douglas C. Morton, Louis Giglio, Ronan Paugam, Yang Chen, Stijn Hantson, Guido R. van der Werf, and James T. Randerson
Earth Syst. Sci. Data, 11, 529–552, https://doi.org/10.5194/essd-11-529-2019, https://doi.org/10.5194/essd-11-529-2019, 2019
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Natural and human-ignited fires affect all major biomes, and satellite observations provide evidence for rapid changes in global fire activity. The Global Fire Atlas of individual fire size, duration, speed, and direction is the first global data product on individual fire behavior. Moving towards a global understanding of individual fire behavior is a critical next step in fire research, required to understand how global fire regimes are changing in response to land management and climate.
Corinne Le Quéré, Robbie M. Andrew, Pierre Friedlingstein, Stephen Sitch, Judith Hauck, Julia Pongratz, Penelope A. Pickers, Jan Ivar Korsbakken, Glen P. Peters, Josep G. Canadell, Almut Arneth, Vivek K. Arora, Leticia Barbero, Ana Bastos, Laurent Bopp, Frédéric Chevallier, Louise P. Chini, Philippe Ciais, Scott C. Doney, Thanos Gkritzalis, Daniel S. Goll, Ian Harris, Vanessa Haverd, Forrest M. Hoffman, Mario Hoppema, Richard A. Houghton, George Hurtt, Tatiana Ilyina, Atul K. Jain, Truls Johannessen, Chris D. Jones, Etsushi Kato, Ralph F. Keeling, Kees Klein Goldewijk, Peter Landschützer, Nathalie Lefèvre, Sebastian Lienert, Zhu Liu, Danica Lombardozzi, Nicolas Metzl, David R. Munro, Julia E. M. S. Nabel, Shin-ichiro Nakaoka, Craig Neill, Are Olsen, Tsueno Ono, Prabir Patra, Anna Peregon, Wouter Peters, Philippe Peylin, Benjamin Pfeil, Denis Pierrot, Benjamin Poulter, Gregor Rehder, Laure Resplandy, Eddy Robertson, Matthias Rocher, Christian Rödenbeck, Ute Schuster, Jörg Schwinger, Roland Séférian, Ingunn Skjelvan, Tobias Steinhoff, Adrienne Sutton, Pieter P. Tans, Hanqin Tian, Bronte Tilbrook, Francesco N. Tubiello, Ingrid T. van der Laan-Luijkx, Guido R. van der Werf, Nicolas Viovy, Anthony P. Walker, Andrew J. Wiltshire, Rebecca Wright, Sönke Zaehle, and Bo Zheng
Earth Syst. Sci. Data, 10, 2141–2194, https://doi.org/10.5194/essd-10-2141-2018, https://doi.org/10.5194/essd-10-2141-2018, 2018
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The Global Carbon Budget 2018 describes the data sets and methodology used to quantify the emissions of carbon dioxide and their partitioning among the atmosphere, land, and ocean. These living data are updated every year to provide the highest transparency and traceability in the reporting of CO2, the key driver of climate change.
Jonathan E. Hickman, Enrico Dammers, Corinne Galy-Lacaux, and Guido R. van der Werf
Atmos. Chem. Phys., 18, 16713–16727, https://doi.org/10.5194/acp-18-16713-2018, https://doi.org/10.5194/acp-18-16713-2018, 2018
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Ammonia gas, which contributes to air pollution, is emitted from soils and combustion. In regions with distinct dry and rainy seasons, the first rainfall events each year trigger biogeochemical activity in soils. We used satellite observations of the atmosphere over the African Sahel savanna ecosystem to show that increases in soil moisture at the onset of the rainy season are responsible for large pulsed emissions of ammonia equal to roughly a fifth of annual ammonia emissions from the region
Haiyan Ni, Ru-Jin Huang, Junji Cao, Weiguo Liu, Ting Zhang, Meng Wang, Harro A. J. Meijer, and Ulrike Dusek
Atmos. Chem. Phys., 18, 16363–16383, https://doi.org/10.5194/acp-18-16363-2018, https://doi.org/10.5194/acp-18-16363-2018, 2018
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Seasonal changes in organic carbon (OC) and elemental carbon (EC) sources in Xi'an, China, are investigated based on measurements of radiocarbon and the stable isotope 13C. Relative contributions to EC from biomass burning, coal combustion, and vehicle emissions change substantially between different seasons. Biomass burning contributes 60 % to the EC increment in winter. Comparing concentrations and sources of primary OC to total OC suggests non-negligible OC loss due to active photochemistry.
Corinne Le Quéré, Robbie M. Andrew, Pierre Friedlingstein, Stephen Sitch, Julia Pongratz, Andrew C. Manning, Jan Ivar Korsbakken, Glen P. Peters, Josep G. Canadell, Robert B. Jackson, Thomas A. Boden, Pieter P. Tans, Oliver D. Andrews, Vivek K. Arora, Dorothee C. E. Bakker, Leticia Barbero, Meike Becker, Richard A. Betts, Laurent Bopp, Frédéric Chevallier, Louise P. Chini, Philippe Ciais, Catherine E. Cosca, Jessica Cross, Kim Currie, Thomas Gasser, Ian Harris, Judith Hauck, Vanessa Haverd, Richard A. Houghton, Christopher W. Hunt, George Hurtt, Tatiana Ilyina, Atul K. Jain, Etsushi Kato, Markus Kautz, Ralph F. Keeling, Kees Klein Goldewijk, Arne Körtzinger, Peter Landschützer, Nathalie Lefèvre, Andrew Lenton, Sebastian Lienert, Ivan Lima, Danica Lombardozzi, Nicolas Metzl, Frank Millero, Pedro M. S. Monteiro, David R. Munro, Julia E. M. S. Nabel, Shin-ichiro Nakaoka, Yukihiro Nojiri, X. Antonio Padin, Anna Peregon, Benjamin Pfeil, Denis Pierrot, Benjamin Poulter, Gregor Rehder, Janet Reimer, Christian Rödenbeck, Jörg Schwinger, Roland Séférian, Ingunn Skjelvan, Benjamin D. Stocker, Hanqin Tian, Bronte Tilbrook, Francesco N. Tubiello, Ingrid T. van der Laan-Luijkx, Guido R. van der Werf, Steven van Heuven, Nicolas Viovy, Nicolas Vuichard, Anthony P. Walker, Andrew J. Watson, Andrew J. Wiltshire, Sönke Zaehle, and Dan Zhu
Earth Syst. Sci. Data, 10, 405–448, https://doi.org/10.5194/essd-10-405-2018, https://doi.org/10.5194/essd-10-405-2018, 2018
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The Global Carbon Budget 2017 describes data sets and methodology to quantify the five major components of the global carbon budget and their uncertainties. It is the 12th annual update and the 6th published in this journal.
Taku Umezawa, Carl A. M. Brenninkmeijer, Thomas Röckmann, Carina van der Veen, Stanley C. Tyler, Ryo Fujita, Shinji Morimoto, Shuji Aoki, Todd Sowers, Jochen Schmitt, Michael Bock, Jonas Beck, Hubertus Fischer, Sylvia E. Michel, Bruce H. Vaughn, John B. Miller, James W. C. White, Gordon Brailsford, Hinrich Schaefer, Peter Sperlich, Willi A. Brand, Michael Rothe, Thomas Blunier, David Lowry, Rebecca E. Fisher, Euan G. Nisbet, Andrew L. Rice, Peter Bergamaschi, Cordelia Veidt, and Ingeborg Levin
Atmos. Meas. Tech., 11, 1207–1231, https://doi.org/10.5194/amt-11-1207-2018, https://doi.org/10.5194/amt-11-1207-2018, 2018
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Isotope measurements are useful for separating different methane sources. However, the lack of widely accepted standards and calibration methods for stable carbon and hydrogen isotopic ratios of methane in air has caused significant measurement offsets among laboratories. We conducted worldwide interlaboratory comparisons, surveyed the literature and assessed them systematically. This study may be of help in future attempts to harmonize data sets of isotopic composition of atmospheric methane.
Thierry Fanin and Guido R. van der Werf
Biogeosciences, 14, 3995–4008, https://doi.org/10.5194/bg-14-3995-2017, https://doi.org/10.5194/bg-14-3995-2017, 2017
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Using night fire detection and rainfall datasets during 1997–2015, we found that the number of night fires detected in 1997 was 2.2 times higher than in 2015, but with a higher fraction of peatland burned in 2015. We also confirmed the non-linearity of rainfall accumulation prior to a fire to indicate a high fire year. The influence of rainfall on the number of yearly fires varies across Indonesia. Southern Sumatra and Kalimantan need 120 days of observations, while northern Sumatra only 30.
Guido R. van der Werf, James T. Randerson, Louis Giglio, Thijs T. van Leeuwen, Yang Chen, Brendan M. Rogers, Mingquan Mu, Margreet J. E. van Marle, Douglas C. Morton, G. James Collatz, Robert J. Yokelson, and Prasad S. Kasibhatla
Earth Syst. Sci. Data, 9, 697–720, https://doi.org/10.5194/essd-9-697-2017, https://doi.org/10.5194/essd-9-697-2017, 2017
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Fires occur in many vegetation types and are sometimes natural but often ignited by humans for various purposes. We have estimated how much area they burn globally and what their emissions are. Total burned area is roughly equivalent to the size of the EU with most fires burning in tropical savannas. Their emissions vary substantially from year to year and contribute to the atmospheric burdens of many trace gases and aerosols. The 20-year dataset is mostly suited for large-scale assessments.
Margreet J. E. van Marle, Silvia Kloster, Brian I. Magi, Jennifer R. Marlon, Anne-Laure Daniau, Robert D. Field, Almut Arneth, Matthew Forrest, Stijn Hantson, Natalie M. Kehrwald, Wolfgang Knorr, Gitta Lasslop, Fang Li, Stéphane Mangeon, Chao Yue, Johannes W. Kaiser, and Guido R. van der Werf
Geosci. Model Dev., 10, 3329–3357, https://doi.org/10.5194/gmd-10-3329-2017, https://doi.org/10.5194/gmd-10-3329-2017, 2017
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Fire emission estimates are a key input dataset for climate models. We have merged satellite information with proxy datasets and fire models to reconstruct fire emissions since 1750 AD. Our dataset indicates that, on a global scale, fire emissions were relatively constant over time. Since roughly 1950, declining emissions from savannas were approximately balanced by increased emissions from tropical deforestation zones.
Jakob Zscheischler, Miguel D. Mahecha, Valerio Avitabile, Leonardo Calle, Nuno Carvalhais, Philippe Ciais, Fabian Gans, Nicolas Gruber, Jens Hartmann, Martin Herold, Kazuhito Ichii, Martin Jung, Peter Landschützer, Goulven G. Laruelle, Ronny Lauerwald, Dario Papale, Philippe Peylin, Benjamin Poulter, Deepak Ray, Pierre Regnier, Christian Rödenbeck, Rosa M. Roman-Cuesta, Christopher Schwalm, Gianluca Tramontana, Alexandra Tyukavina, Riccardo Valentini, Guido van der Werf, Tristram O. West, Julie E. Wolf, and Markus Reichstein
Biogeosciences, 14, 3685–3703, https://doi.org/10.5194/bg-14-3685-2017, https://doi.org/10.5194/bg-14-3685-2017, 2017
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Here we synthesize a wide range of global spatiotemporal observational data on carbon exchanges between the Earth surface and the atmosphere. A key challenge was to consistently combining observational products of terrestrial and aquatic surfaces. Our primary goal is to identify today’s key uncertainties and observational shortcomings that would need to be addressed in future measurement campaigns or expansions of in situ observatories.
Carl Meusinger, Ulrike Dusek, Stephanie M. King, Rupert Holzinger, Thomas Rosenørn, Peter Sperlich, Maxime Julien, Gerald S. Remaud, Merete Bilde, Thomas Röckmann, and Matthew S. Johnson
Atmos. Chem. Phys., 17, 6373–6391, https://doi.org/10.5194/acp-17-6373-2017, https://doi.org/10.5194/acp-17-6373-2017, 2017
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Isotope studies can constrain budgets of secondary organic aerosol (SOA) that is pivotal to air pollution and climate. SOA from α-pinene ozonolysis was found to be enriched in 13C relative to the precursor. The observed difference in 13C between the gas and particle phases may arise from isotope-dependent changes in branching ratios. Alternatively, some gas-phase products involve carbon atoms from highly enriched and depleted sites, giving a non-kinetic origin to the observed fractionations.
Célia J. Sapart, Natalia Shakhova, Igor Semiletov, Joachim Jansen, Sönke Szidat, Denis Kosmach, Oleg Dudarev, Carina van der Veen, Matthias Egger, Valentine Sergienko, Anatoly Salyuk, Vladimir Tumskoy, Jean-Louis Tison, and Thomas Röckmann
Biogeosciences, 14, 2283–2292, https://doi.org/10.5194/bg-14-2283-2017, https://doi.org/10.5194/bg-14-2283-2017, 2017
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The Arctic Ocean, especially the Siberian shelves, overlays large areas of subsea permafrost that is degrading. We show that methane with a biogenic origin is emitted from this permafrost. At locations where bubble plumes have been observed, methane can escape oxidation in the surface sediment and rapidly migrate through the very shallow water column of this region to escape to the atmosphere, generating a positive radiative feedback.
Ulrike Dusek, Regina Hitzenberger, Anne Kasper-Giebl, Magdalena Kistler, Harro A. J. Meijer, Sönke Szidat, Lukas Wacker, Rupert Holzinger, and Thomas Röckmann
Atmos. Chem. Phys., 17, 3233–3251, https://doi.org/10.5194/acp-17-3233-2017, https://doi.org/10.5194/acp-17-3233-2017, 2017
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Measurements of the radioactive carbon isotope 14C allow to identify the sources of aerosol carbon. We report an extensive 14C source apportionment record in the Netherlands with samples covering a whole year. We discovered that long-range transport has a large influence on aerosol carbon levels. Fossil fuel carbon is least influenced by long-range transport and more regional in origin. Biomass burning seems to be a minor source of aerosol carbon in the Netherlands.
Marielle Saunois, Philippe Bousquet, Ben Poulter, Anna Peregon, Philippe Ciais, Josep G. Canadell, Edward J. Dlugokencky, Giuseppe Etiope, David Bastviken, Sander Houweling, Greet Janssens-Maenhout, Francesco N. Tubiello, Simona Castaldi, Robert B. Jackson, Mihai Alexe, Vivek K. Arora, David J. Beerling, Peter Bergamaschi, Donald R. Blake, Gordon Brailsford, Victor Brovkin, Lori Bruhwiler, Cyril Crevoisier, Patrick Crill, Kristofer Covey, Charles Curry, Christian Frankenberg, Nicola Gedney, Lena Höglund-Isaksson, Misa Ishizawa, Akihiko Ito, Fortunat Joos, Heon-Sook Kim, Thomas Kleinen, Paul Krummel, Jean-François Lamarque, Ray Langenfelds, Robin Locatelli, Toshinobu Machida, Shamil Maksyutov, Kyle C. McDonald, Julia Marshall, Joe R. Melton, Isamu Morino, Vaishali Naik, Simon O'Doherty, Frans-Jan W. Parmentier, Prabir K. Patra, Changhui Peng, Shushi Peng, Glen P. Peters, Isabelle Pison, Catherine Prigent, Ronald Prinn, Michel Ramonet, William J. Riley, Makoto Saito, Monia Santini, Ronny Schroeder, Isobel J. Simpson, Renato Spahni, Paul Steele, Atsushi Takizawa, Brett F. Thornton, Hanqin Tian, Yasunori Tohjima, Nicolas Viovy, Apostolos Voulgarakis, Michiel van Weele, Guido R. van der Werf, Ray Weiss, Christine Wiedinmyer, David J. Wilton, Andy Wiltshire, Doug Worthy, Debra Wunch, Xiyan Xu, Yukio Yoshida, Bowen Zhang, Zhen Zhang, and Qiuan Zhu
Earth Syst. Sci. Data, 8, 697–751, https://doi.org/10.5194/essd-8-697-2016, https://doi.org/10.5194/essd-8-697-2016, 2016
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An accurate assessment of the methane budget is important to understand the atmospheric methane concentrations and trends and to provide realistic pathways for climate change mitigation. The various and diffuse sources of methane as well and its oxidation by a very short lifetime radical challenge this assessment. We quantify the methane sources and sinks as well as their uncertainties based on both bottom-up and top-down approaches provided by a broad international scientific community.
Dorota Janina Mrozek, Carina van der Veen, Magdalena E. G. Hofmann, Huilin Chen, Rigel Kivi, Pauli Heikkinen, and Thomas Röckmann
Atmos. Meas. Tech., 9, 5607–5620, https://doi.org/10.5194/amt-9-5607-2016, https://doi.org/10.5194/amt-9-5607-2016, 2016
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Stratospheric Air Sub-sampler (SAS) is a device to collect and to store the stratospheric profile of air collected with an AirCore (Karion et al., 2010) in numerous sub-samples. The sub-samples (each of 25 mL at ambient temperature and pressure) can be later introduced to the continuous flow systems to measure for example the isotopic composition of CO2. The performance of the coupled system is demonstrated for a set of air samples from an AirCore flight in November 2014 near Sodankylä, Finland.
Beatriz Sayuri Oyama, Maria de Fátima Andrade, Pierre Herckes, Ulrike Dusek, Thomas Röckmann, and Rupert Holzinger
Atmos. Chem. Phys., 16, 14397–14408, https://doi.org/10.5194/acp-16-14397-2016, https://doi.org/10.5194/acp-16-14397-2016, 2016
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Vehicular emissions have a strong impact on air pollution in big cities; hence, the study was performed in São Paulo city, where light- (LDVs) and heavy-duty vehicles (HDVs) run on different fuels. We find that organic aerosol emission from LDVs and HDVs is a complex process involving oxidation of fuel constituents, NOx chemistry, and condensation of unburned fuel hydrocarbons on new or existing particles. The obtained emission patterns can be used to study processing of young aerosol in Brazil.
Corinne Le Quéré, Robbie M. Andrew, Josep G. Canadell, Stephen Sitch, Jan Ivar Korsbakken, Glen P. Peters, Andrew C. Manning, Thomas A. Boden, Pieter P. Tans, Richard A. Houghton, Ralph F. Keeling, Simone Alin, Oliver D. Andrews, Peter Anthoni, Leticia Barbero, Laurent Bopp, Frédéric Chevallier, Louise P. Chini, Philippe Ciais, Kim Currie, Christine Delire, Scott C. Doney, Pierre Friedlingstein, Thanos Gkritzalis, Ian Harris, Judith Hauck, Vanessa Haverd, Mario Hoppema, Kees Klein Goldewijk, Atul K. Jain, Etsushi Kato, Arne Körtzinger, Peter Landschützer, Nathalie Lefèvre, Andrew Lenton, Sebastian Lienert, Danica Lombardozzi, Joe R. Melton, Nicolas Metzl, Frank Millero, Pedro M. S. Monteiro, David R. Munro, Julia E. M. S. Nabel, Shin-ichiro Nakaoka, Kevin O'Brien, Are Olsen, Abdirahman M. Omar, Tsuneo Ono, Denis Pierrot, Benjamin Poulter, Christian Rödenbeck, Joe Salisbury, Ute Schuster, Jörg Schwinger, Roland Séférian, Ingunn Skjelvan, Benjamin D. Stocker, Adrienne J. Sutton, Taro Takahashi, Hanqin Tian, Bronte Tilbrook, Ingrid T. van der Laan-Luijkx, Guido R. van der Werf, Nicolas Viovy, Anthony P. Walker, Andrew J. Wiltshire, and Sönke Zaehle
Earth Syst. Sci. Data, 8, 605–649, https://doi.org/10.5194/essd-8-605-2016, https://doi.org/10.5194/essd-8-605-2016, 2016
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The Global Carbon Budget 2016 is the 11th annual update of emissions of carbon dioxide (CO2) and their partitioning among the atmosphere, land, and ocean. This data synthesis brings together measurements, statistical information, and analyses of model results in order to provide an assessment of the global carbon budget and their uncertainties for years 1959 to 2015, with a projection for year 2016.
Thomas Röckmann, Simon Eyer, Carina van der Veen, Maria E. Popa, Béla Tuzson, Guillaume Monteil, Sander Houweling, Eliza Harris, Dominik Brunner, Hubertus Fischer, Giulia Zazzeri, David Lowry, Euan G. Nisbet, Willi A. Brand, Jaroslav M. Necki, Lukas Emmenegger, and Joachim Mohn
Atmos. Chem. Phys., 16, 10469–10487, https://doi.org/10.5194/acp-16-10469-2016, https://doi.org/10.5194/acp-16-10469-2016, 2016
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A dual isotope ratio mass spectrometric system (IRMS) and a quantum cascade laser absorption spectroscopy (QCLAS)-based technique were deployed at the Cabauw experimental site for atmospheric research (CESAR) in the Netherlands and performed in situ, high-frequency (approx. hourly) measurements for a period of more than 5 months, yielding a combined dataset with more than 2500 measurements of both δ13C and δD.
Peter Sperlich, Nelly A. M. Uitslag, Jürgen M. Richter, Michael Rothe, Heike Geilmann, Carina van der Veen, Thomas Röckmann, Thomas Blunier, and Willi A. Brand
Atmos. Meas. Tech., 9, 3717–3737, https://doi.org/10.5194/amt-9-3717-2016, https://doi.org/10.5194/amt-9-3717-2016, 2016
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Isotope measurements in atmospheric CH4 are performed since more than 3 decades. However, standard gases to harmonize global measurements are not available to this day. We designed two methods to calibrate a suite of 8 CH4 gases with a wide range in isotopic composition to the VPDB and VSMOW scales with high precision and accuracy. Synthetic air mixtures with ~2 ppm of calibrated CH4 can be provided to the community by the ISOLAB of the Max Planck Institute for Biogeochemistry in Jena, Germany.
Niels Andela, Guido R. van der Werf, Johannes W. Kaiser, Thijs T. van Leeuwen, Martin J. Wooster, and Caroline E. R. Lehmann
Biogeosciences, 13, 3717–3734, https://doi.org/10.5194/bg-13-3717-2016, https://doi.org/10.5194/bg-13-3717-2016, 2016
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Landscape fires occur on a large scale in savannas and grasslands, affecting ecosystems and air quality. We combined two satellite-derived datasets to derive fuel consumption per unit of area burned for savannas and grasslands in the (sub)tropics. Fire return periods, vegetation productivity, vegetation type and human land management were all important drivers of its spatial distribution. The results can be used to improve fire emission modelling and management or to detect ecosystem degradation.
Stijn Hantson, Almut Arneth, Sandy P. Harrison, Douglas I. Kelley, I. Colin Prentice, Sam S. Rabin, Sally Archibald, Florent Mouillot, Steve R. Arnold, Paulo Artaxo, Dominique Bachelet, Philippe Ciais, Matthew Forrest, Pierre Friedlingstein, Thomas Hickler, Jed O. Kaplan, Silvia Kloster, Wolfgang Knorr, Gitta Lasslop, Fang Li, Stephane Mangeon, Joe R. Melton, Andrea Meyn, Stephen Sitch, Allan Spessa, Guido R. van der Werf, Apostolos Voulgarakis, and Chao Yue
Biogeosciences, 13, 3359–3375, https://doi.org/10.5194/bg-13-3359-2016, https://doi.org/10.5194/bg-13-3359-2016, 2016
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Our ability to predict the magnitude and geographic pattern of past and future fire impacts rests on our ability to model fire regimes. A large variety of models exist, and it is unclear which type of model or degree of complexity is required to model fire adequately at regional to global scales. In this paper we summarize the current state of the art in fire-regime modelling and model evaluation, and outline what lessons may be learned from the Fire Model Intercomparison Project – FireMIP.
M. J. E. van Marle, G. R. van der Werf, R. A. M. de Jeu, and Y. Y. Liu
Biogeosciences, 13, 609–624, https://doi.org/10.5194/bg-13-609-2016, https://doi.org/10.5194/bg-13-609-2016, 2016
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We have quantified large-scale forest loss over a 21-year period (1990–2010) in the tropical biomes of South America using a new satellite-based data set. We found that South American forest exhibited interannual variability without a clear trend during the 1990s, but increased from 2000 to 2004. After 2004, forest loss decreased again, mainly as a result of a decrease in the Brazilian Amazon, whereas at the same time regions south of the arc of deforestation showed an increase in forest loss.
S. Eyer, B. Tuzson, M. E. Popa, C. van der Veen, T. Röckmann, M. Rothe, W. A. Brand, R. Fisher, D. Lowry, E. G. Nisbet, M. S. Brennwald, E. Harris, C. Zellweger, L. Emmenegger, H. Fischer, and J. Mohn
Atmos. Meas. Tech., 9, 263–280, https://doi.org/10.5194/amt-9-263-2016, https://doi.org/10.5194/amt-9-263-2016, 2016
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We present a newly developed field-deployable, autonomous platform simultaneously measuring the three most abundant isotopologues of methane using mid-infrared laser absorption spectroscopy.
The instrument consists of a compact quantum cascade laser absorption spectrometer (QCLAS) coupled to a preconcentration unit, called TRace gas EXtractor (TREX).
The performance of this new in situ technique was investigated during a 2-week measurement campaign and compared to other techniques.
S. Walter, A. Kock, T. Steinhoff, B. Fiedler, P. Fietzek, J. Kaiser, M. Krol, M. E. Popa, Q. Chen, T. Tanhua, and T. Röckmann
Biogeosciences, 13, 323–340, https://doi.org/10.5194/bg-13-323-2016, https://doi.org/10.5194/bg-13-323-2016, 2016
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Oceans are a source of H2, an indirect greenhouse gas. Measurements constraining the temporal and spatial patterns of oceanic H2 emissions are sparse and although H2 is assumed to be produced mainly biologically, direct evidence for biogenic marine production was lacking. By analyzing the H2 isotopic composition (δD) we were able to constrain the global H2 budget in more detail, verify biogenic production and point to additional sources. We also showed that current models are reasonably working.
S. L. Pathirana, C. van der Veen, M. E. Popa, and T. Röckmann
Atmos. Meas. Tech., 8, 5315–5324, https://doi.org/10.5194/amt-8-5315-2015, https://doi.org/10.5194/amt-8-5315-2015, 2015
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CO is established as an important indirect greenhouse gas, as it is the major sink for the OH∙. We have developed a fully automated system for the determination of δ13C and δ18O in atmospheric CO. The blank signal of the Schütze reagent is 1-3 % of the typical sample size. The repeatability is 0.1 ‰ for δ13C and 0.2 ‰ for δ18O. The analytical repeatability for the mole fraction is ~0.7 nmol mol-1 for 100 mL of ambient air (185.4 nmol mol-1 of CO). A single measurement is performed in 18 min.
C. Le Quéré, R. Moriarty, R. M. Andrew, J. G. Canadell, S. Sitch, J. I. Korsbakken, P. Friedlingstein, G. P. Peters, R. J. Andres, T. A. Boden, R. A. Houghton, J. I. House, R. F. Keeling, P. Tans, A. Arneth, D. C. E. Bakker, L. Barbero, L. Bopp, J. Chang, F. Chevallier, L. P. Chini, P. Ciais, M. Fader, R. A. Feely, T. Gkritzalis, I. Harris, J. Hauck, T. Ilyina, A. K. Jain, E. Kato, V. Kitidis, K. Klein Goldewijk, C. Koven, P. Landschützer, S. K. Lauvset, N. Lefèvre, A. Lenton, I. D. Lima, N. Metzl, F. Millero, D. R. Munro, A. Murata, J. E. M. S. Nabel, S. Nakaoka, Y. Nojiri, K. O'Brien, A. Olsen, T. Ono, F. F. Pérez, B. Pfeil, D. Pierrot, B. Poulter, G. Rehder, C. Rödenbeck, S. Saito, U. Schuster, J. Schwinger, R. Séférian, T. Steinhoff, B. D. Stocker, A. J. Sutton, T. Takahashi, B. Tilbrook, I. T. van der Laan-Luijkx, G. R. van der Werf, S. van Heuven, D. Vandemark, N. Viovy, A. Wiltshire, S. Zaehle, and N. Zeng
Earth Syst. Sci. Data, 7, 349–396, https://doi.org/10.5194/essd-7-349-2015, https://doi.org/10.5194/essd-7-349-2015, 2015
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Accurate assessment of anthropogenic carbon dioxide emissions and their redistribution among the atmosphere, ocean, and terrestrial biosphere is important to understand the global carbon cycle, support the development of climate policies, and project future climate change. We describe data sets and a methodology to quantify all major components of the global carbon budget, including their uncertainties, based on a range of data and models and their interpretation by a broad scientific community.
Q. Chen, M. E. Popa, A. M. Batenburg, and T. Röckmann
Atmos. Chem. Phys., 15, 13003–13021, https://doi.org/10.5194/acp-15-13003-2015, https://doi.org/10.5194/acp-15-13003-2015, 2015
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We investigated soil production and uptake of H2 and associated isotope effects. Uptake and emission of H2 occurred simultaneously at all sampling sites, with strongest emission where N2 fixing legume was present. The fractionation constant during soil uptake was about 0.945 and it did not show positive correlation with deposition velocity. The isotopic composition of H2 emitted from soil with legume was about -530‰, which is less deuterium-depleted than isotope equilibrium between H2O and H2.
T. Fanin and G. R. van der Werf
Biogeosciences, 12, 6033–6043, https://doi.org/10.5194/bg-12-6033-2015, https://doi.org/10.5194/bg-12-6033-2015, 2015
N. Andela, J. W. Kaiser, G. R. van der Werf, and M. J. Wooster
Atmos. Chem. Phys., 15, 8831–8846, https://doi.org/10.5194/acp-15-8831-2015, https://doi.org/10.5194/acp-15-8831-2015, 2015
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The polar orbiting MODIS instruments provide four daily observations of the fire diurnal cycle, resulting in erroneous fire radiative energy (FRE) estimates. Using geostationary SEVIRI data, we explore the fire diurnal cycle and its drivers for Africa to develop a new method to estimate global FRE in near real-time using MODIS. The fire diurnal cycle varied with climate and vegetation type, and including information on the fire diurnal cycle in the model significantly improved the FRE estimates.
C. Le Quéré, R. Moriarty, R. M. Andrew, G. P. Peters, P. Ciais, P. Friedlingstein, S. D. Jones, S. Sitch, P. Tans, A. Arneth, T. A. Boden, L. Bopp, Y. Bozec, J. G. Canadell, L. P. Chini, F. Chevallier, C. E. Cosca, I. Harris, M. Hoppema, R. A. Houghton, J. I. House, A. K. Jain, T. Johannessen, E. Kato, R. F. Keeling, V. Kitidis, K. Klein Goldewijk, C. Koven, C. S. Landa, P. Landschützer, A. Lenton, I. D. Lima, G. Marland, J. T. Mathis, N. Metzl, Y. Nojiri, A. Olsen, T. Ono, S. Peng, W. Peters, B. Pfeil, B. Poulter, M. R. Raupach, P. Regnier, C. Rödenbeck, S. Saito, J. E. Salisbury, U. Schuster, J. Schwinger, R. Séférian, J. Segschneider, T. Steinhoff, B. D. Stocker, A. J. Sutton, T. Takahashi, B. Tilbrook, G. R. van der Werf, N. Viovy, Y.-P. Wang, R. Wanninkhof, A. Wiltshire, and N. Zeng
Earth Syst. Sci. Data, 7, 47–85, https://doi.org/10.5194/essd-7-47-2015, https://doi.org/10.5194/essd-7-47-2015, 2015
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Carbon dioxide (CO2) emissions from human activities (burning fossil fuels and cement production, deforestation and other land-use change) are set to rise again in 2014.
This study (updated yearly) makes an accurate assessment of anthropogenic CO2 emissions and their redistribution between the atmosphere, ocean, and terrestrial biosphere in order to better understand the global carbon cycle, support the development of climate policies, and project future climate change.
B. Aouizerats, G. R. van der Werf, R. Balasubramanian, and R. Betha
Atmos. Chem. Phys., 15, 363–373, https://doi.org/10.5194/acp-15-363-2015, https://doi.org/10.5194/acp-15-363-2015, 2015
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In this study, we simulated the regional transport and evolution of biomass burning occurring in Indonesia during the high fire event in 2006.
We studied and quantified the contribution of those fires to the Singapore pollution levels.
This high resolution modelling study showed that about half of the particulate pollution events in Singapore were mainly due to fires occurring in Sumatra (Indonesia), while the other half were due to local pollution.
T. T. van Leeuwen, G. R. van der Werf, A. A. Hoffmann, R. G. Detmers, G. Rücker, N. H. F. French, S. Archibald, J. A. Carvalho Jr., G. D. Cook, W. J. de Groot, C. Hély, E. S. Kasischke, S. Kloster, J. L. McCarty, M. L. Pettinari, P. Savadogo, E. C. Alvarado, L. Boschetti, S. Manuri, C. P. Meyer, F. Siegert, L. A. Trollope, and W. S. W. Trollope
Biogeosciences, 11, 7305–7329, https://doi.org/10.5194/bg-11-7305-2014, https://doi.org/10.5194/bg-11-7305-2014, 2014
I. R. van der Velde, J. B. Miller, K. Schaefer, G. R. van der Werf, M. C. Krol, and W. Peters
Biogeosciences, 11, 6553–6571, https://doi.org/10.5194/bg-11-6553-2014, https://doi.org/10.5194/bg-11-6553-2014, 2014
G. R. van der Werf and A. J. Dolman
Earth Syst. Dynam., 5, 375–382, https://doi.org/10.5194/esd-5-375-2014, https://doi.org/10.5194/esd-5-375-2014, 2014
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Climate sensitivity can be quantified using measured changes in temperature and forcings. This approach requires disentangling natural and anthropogenic influences on global climate. We focused on the role of the Atlantic Multidecadal Oscillation (AMO) in this and show how different AMO characterizations influence the anthropogenic temperature trends (we found they were in between previously published values) and transient climate sensitivity, which we found to be 1.6 (1.0-3.3)°C.
U. Dusek, M. Monaco, M. Prokopiou, F. Gongriep, R. Hitzenberger, H. A. J. Meijer, and T. Röckmann
Atmos. Meas. Tech., 7, 1943–1955, https://doi.org/10.5194/amt-7-1943-2014, https://doi.org/10.5194/amt-7-1943-2014, 2014
R. L. Thompson, K. Ishijima, E. Saikawa, M. Corazza, U. Karstens, P. K. Patra, P. Bergamaschi, F. Chevallier, E. Dlugokencky, R. G. Prinn, R. F. Weiss, S. O'Doherty, P. J. Fraser, L. P. Steele, P. B. Krummel, A. Vermeulen, Y. Tohjima, A. Jordan, L. Haszpra, M. Steinbacher, S. Van der Laan, T. Aalto, F. Meinhardt, M. E. Popa, J. Moncrieff, and P. Bousquet
Atmos. Chem. Phys., 14, 6177–6194, https://doi.org/10.5194/acp-14-6177-2014, https://doi.org/10.5194/acp-14-6177-2014, 2014
P. Castellanos, K. F. Boersma, and G. R. van der Werf
Atmos. Chem. Phys., 14, 3929–3943, https://doi.org/10.5194/acp-14-3929-2014, https://doi.org/10.5194/acp-14-3929-2014, 2014
M. E. Popa, M. K. Vollmer, A. Jordan, W. A. Brand, S. L. Pathirana, M. Rothe, and T. Röckmann
Atmos. Chem. Phys., 14, 2105–2123, https://doi.org/10.5194/acp-14-2105-2014, https://doi.org/10.5194/acp-14-2105-2014, 2014
Related subject area
Subject: Gases | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Impact of HO2∕RO2 ratio on highly oxygenated α-pinene photooxidation products and secondary organic aerosol formation potential
Negligible temperature dependence of the ozone–iodide reaction and implications for oceanic emissions of iodine
Extension, development, and evaluation of the representation of the OH-initiated dimethyl sulfide (DMS) oxidation mechanism in the Master Chemical Mechanism (MCM) v3.3.1 framework
On the potential use of highly oxygenated organic molecules (HOMs) as indicators for ozone formation sensitivity
Oxygenated organic molecules produced by low-NOx photooxidation of aromatic compounds: contributions to secondary organic aerosol and steric hindrance
Impact of temperature on the role of Criegee intermediates and peroxy radicals in dimer formation from β-pinene ozonolysis
Atmospheric impact of 2-methylpentanal emissions: kinetics, photochemistry, and formation of secondary pollutants
Technical note: Gas-phase nitrate radical generation via irradiation of aerated ceric ammonium nitrate mixtures
Direct probing of acylperoxy radicals during ozonolysis of α-pinene: constraints on radical chemistry and production of highly oxygenated organic molecules
Atmospheric photooxidation and ozonolysis of sabinene: reaction rate coefficients, product yields, and chemical budget of radicals
Compilation of Henry's law constants (version 5.0.0) for water as solvent
Measurement report: Carbonyl sulfide production during dimethyl sulfide oxidation in the atmospheric simulation chamber SAPHIR
An aldehyde as a rapid source of secondary aerosol precursors: theoretical and experimental study of hexanal autoxidation
Measuring and modeling investigation of the net photochemical ozone production rate via an improved dual-channel reaction chamber technique
Secondary reactions of aromatics-derived oxygenated organic molecules lead to plentiful highly oxygenated organic molecules within an intraday OH exposure
Evolution of organic carbon in the laboratory oxidation of biomass-burning emissions
Atmospheric oxidation of new “green” solvents – Part 2: methyl pivalate and pinacolone
On the formation of highly oxidized pollutants by autoxidation of terpenes under low-temperature-combustion conditions: the case of limonene and α-pinene
Selective deuteration as a tool for resolving autoxidation mechanisms in α-pinene ozonolysis
Comparison of isoprene chemical mechanisms under atmospheric night-time conditions in chamber experiments: evidence of hydroperoxy aldehydes and epoxy products from NO3 oxidation
Measurement of Henry's law and liquid-phase loss rate constants of peroxypropionic nitric anhydride (PPN) in deionized water and in n-octanol
Product distribution, kinetics, and aerosol formation from the OH oxidation of dimethyl sulfide under different RO2 regimes
Atmospheric breakdown chemistry of the new “green” solvent 2,2,5,5-tetramethyloxolane via gas-phase reactions with OH and Cl radicals
Impact of cooking style and oil on semi-volatile and intermediate volatility organic compound emissions from Chinese domestic cooking
Observations of gas-phase products from the nitrate-radical-initiated oxidation of four monoterpenes
Investigation of the limonene photooxidation by OH at different NO concentrations in the atmospheric simulation chamber SAPHIR (Simulation of Atmospheric PHotochemistry In a large Reaction Chamber)
Kinetic study of the atmospheric oxidation of a series of epoxy compounds by OH radicals
An experimental study of the reactivity of terpinolene and β-caryophyllene with the nitrate radical
Oxidation product characterization from ozonolysis of the diterpene ent-kaurene
Kinetics of OH + SO2 + M: temperature-dependent rate coefficients in the fall-off regime and the influence of water vapour
Formation of organic sulfur compounds through SO2-initiated photochemistry of PAHs and dimethylsulfoxide at the air-water interface
Evaluation of the daytime tropospheric loss of 2-methylbutanal
Investigations into the gas-phase photolysis and OH radical kinetics of nitrocatechols: implications of intramolecular interactions on their atmospheric behaviour
Reproducing Arctic springtime tropospheric ozone and mercury depletion events in an outdoor mesocosm sea ice facility
N2O5 uptake onto saline mineral dust: a potential missing source of tropospheric ClNO2 in inland China
NO3 chemistry of wildfire emissions: a kinetic study of the gas-phase reactions of furans with the NO3 radical
Marine gas-phase sulfur emissions during an induced phytoplankton bloom
Biomass burning plume chemistry: OH-radical-initiated oxidation of 3-penten-2-one and its main oxidation product 2-hydroxypropanal
Atmospheric photo-oxidation of myrcene: OH reaction rate constant, gas-phase oxidation products and radical budgets
Characterization of ambient volatile organic compounds, source apportionment, and the ozone–NOx–VOC sensitivities in a heavily polluted megacity of central China: effect of sporting events and emission reductions
Atmospheric oxidation of α,β-unsaturated ketones: kinetics and mechanism of the OH radical reaction
Reactions of NO3 with aromatic aldehydes: gas-phase kinetics and insights into the mechanism of the reaction
Atmospheric photooxidation and ozonolysis of Δ3-carene and 3-caronaldehyde: rate constants and product yields
Measurement report: Biogenic volatile organic compound emission profiles of rapeseed leaf litter and its secondary organic aerosol formation potential
Highly oxygenated organic molecules produced by the oxidation of benzene and toluene in a wide range of OH exposure and NOx conditions
Molecular composition and volatility of multi-generation products formed from isoprene oxidation by nitrate radical
Highly oxygenated organic molecule (HOM) formation in the isoprene oxidation by NO3 radical
Volatile organic compound emissions from solvent- and water-borne coatings – compositional differences and tracer compound identifications
Evaluated kinetic and photochemical data for atmospheric chemistry: volume VIII – gas-phase reactions of organic species with four, or more, carbon atoms ( ≥ C4)
Chemical characterisation of benzene oxidation products under high- and low-NOx conditions using chemical ionisation mass spectrometry
Yarê Baker, Sungah Kang, Hui Wang, Rongrong Wu, Jian Xu, Annika Zanders, Quanfu He, Thorsten Hohaus, Till Ziehm, Veronica Geretti, Thomas J. Bannan, Simon P. O'Meara, Aristeidis Voliotis, Mattias Hallquist, Gordon McFiggans, Sören R. Zorn, Andreas Wahner, and Thomas F. Mentel
Atmos. Chem. Phys., 24, 4789–4807, https://doi.org/10.5194/acp-24-4789-2024, https://doi.org/10.5194/acp-24-4789-2024, 2024
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Highly oxygenated organic molecules are important contributors to secondary organic aerosol. Their yield depends on detailed atmospheric chemical composition. One important parameter is the ratio of hydroperoxy radicals to organic peroxy radicals (HO2/RO2), and we show that higher HO2/RO2 ratios lower the secondary organic aerosol yield. This is of importance as laboratory studies are often biased towards organic peroxy radicals.
Lucy V. Brown, Ryan J. Pound, Lyndsay S. Ives, Matthew R. Jones, Stephen J. Andrews, and Lucy J. Carpenter
Atmos. Chem. Phys., 24, 3905–3923, https://doi.org/10.5194/acp-24-3905-2024, https://doi.org/10.5194/acp-24-3905-2024, 2024
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Ozone is deposited from the lower atmosphere to the surface of the ocean; however, the chemical reactions which drive this deposition are currently not well understood. Of particular importance is the reaction between ozone and iodide, and this work measures the kinetics of this reaction and its temperature dependence, which we find to be negligible. We then investigate the subsequent emissions of iodine-containing species from the surface ocean, which can further impact ozone.
Lorrie Simone Denise Jacob, Chiara Giorio, and Alexander Thomas Archibald
Atmos. Chem. Phys., 24, 3329–3347, https://doi.org/10.5194/acp-24-3329-2024, https://doi.org/10.5194/acp-24-3329-2024, 2024
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Recent studies on DMS have provided new challenges to our mechanistic understanding. Here we synthesise a number of recent studies to further develop and extend a state-of-the-art mechanism. Our new mechanism is shown to outperform all existing mechanisms when compared over a wide set of conditions. The development of an improved DMS mechanism will help lead the way to better the understanding the climate impacts of DMS emissions in past, present, and future atmospheric conditions.
Jiangyi Zhang, Jian Zhao, Yuanyuan Luo, Valter Mickwitz, Douglas Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 24, 2885–2911, https://doi.org/10.5194/acp-24-2885-2024, https://doi.org/10.5194/acp-24-2885-2024, 2024
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Due to the intrinsic connection between the formation pathways of O3 and HOMs, the ratio of HOM dimers or non-nitrate monomers to HOM organic nitrates could be used to determine O3 formation regimes. Owing to the fast formation and short lifetimes of HOMs, HOM-based indicating ratios can describe O3 formation in real time. Despite the success of our approach in this simple laboratory system, applicability to the much more complex atmosphere remains to be determined.
Xi Cheng, Yong Jie Li, Yan Zheng, Keren Liao, Theodore K. Koenig, Yanli Ge, Tong Zhu, Chunxiang Ye, Xinghua Qiu, and Qi Chen
Atmos. Chem. Phys., 24, 2099–2112, https://doi.org/10.5194/acp-24-2099-2024, https://doi.org/10.5194/acp-24-2099-2024, 2024
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In this study we conducted laboratory measurements to investigate the formation of gas-phase oxygenated organic molecules (OOMs) from six aromatic volatile organic compounds (VOCs). We provide a thorough analysis on the effects of precursor structure (substituents and ring numbers) on product distribution and highlight from a laboratory perspective that heavy (e.g., double-ring) aromatic VOCs are important in initial particle growth during secondary organic aerosol formation.
Yiwei Gong, Feng Jiang, Yanxia Li, Thomas Leisner, and Harald Saathoff
Atmos. Chem. Phys., 24, 167–184, https://doi.org/10.5194/acp-24-167-2024, https://doi.org/10.5194/acp-24-167-2024, 2024
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This study investigates the role of the important atmospheric reactive intermediates in the formation of dimers and aerosol in monoterpene ozonolysis at different temperatures. Through conducting a series of chamber experiments and utilizing chemical kinetic and aerosol dynamic models, the SOA formation processes are better described, especially for colder regions. The results can be used to improve the chemical mechanism modeling of monoterpenes and SOA parameterization in transport models.
María Asensio, Sergio Blázquez, María Antiñolo, José Albaladejo, and Elena Jiménez
Atmos. Chem. Phys., 23, 14115–14126, https://doi.org/10.5194/acp-23-14115-2023, https://doi.org/10.5194/acp-23-14115-2023, 2023
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In this work, we focus on the atmospheric chemistry and consequences for air quality of 2-methylpentanal (2MP), which is widely used as a flavoring ingredient and as an intermediate in the synthesis of dyes, resins, and pharmaceuticals. Measurements are presented on how fast 2MP is degraded by sunlight and oxidants like hydroxyl (OH) radicals and chlorine (Cl) atoms and what products are generated. We conclude that 2MP will be degraded in a few hours, affecting local air quality.
Andrew T. Lambe, Bin Bai, Masayuki Takeuchi, Nicole Orwat, Paul M. Zimmerman, Mitchell W. Alton, Nga L. Ng, Andrew Freedman, Megan S. Claflin, Drew R. Gentner, Douglas R. Worsnop, and Pengfei Liu
Atmos. Chem. Phys., 23, 13869–13882, https://doi.org/10.5194/acp-23-13869-2023, https://doi.org/10.5194/acp-23-13869-2023, 2023
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We developed a new method to generate nitrate radicals (NO3) for atmospheric chemistry applications that works by irradiating mixtures containing ceric ammonium nitrate with a UV light at room temperature. It has several advantages over traditional NO3 sources. We characterized its performance over a range of mixture and reactor conditions as well as other irradiation products. Proof of concept was demonstrated by generating and characterizing oxidation products of the β-pinene + NO3 reaction.
Han Zang, Dandan Huang, Jiali Zhong, Ziyue Li, Chenxi Li, Huayun Xiao, and Yue Zhao
Atmos. Chem. Phys., 23, 12691–12705, https://doi.org/10.5194/acp-23-12691-2023, https://doi.org/10.5194/acp-23-12691-2023, 2023
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Acylperoxy radicals (RO2) are key intermediates in the atmospheric oxidation of organic compounds, yet our knowledge of their identities and chemistry remains poor. Using direct measurements and kinetic modeling, we identify the composition and formation pathways of acyl RO2 and quantify their contribution to highly oxygenated organic molecules during α-pinene ozonolysis, which will help to understand oxidation chemistry of monoterpenes and sources of low-volatility organics in the atmosphere.
Jacky Y. S. Pang, Florian Berg, Anna Novelli, Birger Bohn, Michelle Färber, Philip T. M. Carlsson, René Dubus, Georgios I. Gkatzelis, Franz Rohrer, Sergej Wedel, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 23, 12631–12649, https://doi.org/10.5194/acp-23-12631-2023, https://doi.org/10.5194/acp-23-12631-2023, 2023
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In this study, the oxidations of sabinene by OH radicals and ozone were investigated with an atmospheric simulation chamber. Reaction rate coefficients of the OH-oxidation reaction at temperatures between 284 to 340 K were determined for the first time in the laboratory by measuring the OH reactivity. Product yields determined in chamber experiments had good agreement with literature values, but discrepancies were found between experimental yields and expected yields from oxidation mechanisms.
Rolf Sander
Atmos. Chem. Phys., 23, 10901–12440, https://doi.org/10.5194/acp-23-10901-2023, https://doi.org/10.5194/acp-23-10901-2023, 2023
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According to Henry's law, the equilibrium ratio between the abundances in the gas phase and in the aqueous phase is constant for a dilute solution. Henry’s law constants of trace gases of potential importance in environmental chemistry have been collected and converted into a uniform format. The compilation contains 46 434 values of Henry's law constants for 10 173 species, collected from 995 references. It is also available on the internet at https://www.henrys-law.org.
Marc von Hobe, Domenico Taraborrelli, Sascha Alber, Birger Bohn, Hans-Peter Dorn, Hendrik Fuchs, Yun Li, Chenxi Qiu, Franz Rohrer, Roberto Sommariva, Fred Stroh, Zhaofeng Tan, Sergej Wedel, and Anna Novelli
Atmos. Chem. Phys., 23, 10609–10623, https://doi.org/10.5194/acp-23-10609-2023, https://doi.org/10.5194/acp-23-10609-2023, 2023
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The trace gas carbonyl sulfide (OCS) transports sulfur from the troposphere to the stratosphere, where sulfate aerosols are formed that influence climate and stratospheric chemistry. An uncertain OCS source in the troposphere is chemical production form dimethyl sulfide (DMS), a gas released in large quantities from the oceans. We carried out experiments in a large atmospheric simulation chamber to further elucidate the chemical mechanism of OCS production from DMS.
Shawon Barua, Siddharth Iyer, Avinash Kumar, Prasenjit Seal, and Matti Rissanen
Atmos. Chem. Phys., 23, 10517–10532, https://doi.org/10.5194/acp-23-10517-2023, https://doi.org/10.5194/acp-23-10517-2023, 2023
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This work illustrates how a common volatile hydrocarbon, hexanal, has the potential to undergo atmospheric autoxidation that leads to prompt formation of condensable material that subsequently contributes to aerosol formation, deteriorating the air quality of urban atmospheres. We used the combined state-of-the-art quantum chemical modeling and experimental flow reactor experiments under atmospheric conditions to resolve the autoxidation mechanism of hexanal initiated by a common oxidant.
Yixin Hao, Jun Zhou, Jie-Ping Zhou, Yan Wang, Suxia Yang, Yibo Huangfu, Xiao-Bing Li, Chunsheng Zhang, Aiming Liu, Yanfeng Wu, Yaqing Zhou, Shuchun Yang, Yuwen Peng, Jipeng Qi, Xianjun He, Xin Song, Yubin Chen, Bin Yuan, and Min Shao
Atmos. Chem. Phys., 23, 9891–9910, https://doi.org/10.5194/acp-23-9891-2023, https://doi.org/10.5194/acp-23-9891-2023, 2023
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By employing an improved net photochemical ozone production rate (NPOPR) detection system based on the dual-channel reaction chamber technique, we measured the net photochemical ozone production rate in the Pearl River Delta in China. The photochemical ozone formation mechanisms in the reaction and reference chambers were investigated using the observation-data-constrained box model, which helped us to validate the NPOPR detection system and understand photochemical ozone formation mechanism.
Yuwei Wang, Yueyang Li, Gan Yang, Xueyan Yang, Yizhen Wu, Chuang Li, Lei Yao, Hefeng Zhang, and Lin Wang
EGUsphere, https://doi.org/10.5194/egusphere-2023-1702, https://doi.org/10.5194/egusphere-2023-1702, 2023
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The formation and evolution mechanisms of aromatics-derived highly oxygenated organic molecules (HOMs) is essential to understanding the formation of secondary organic aerosol pollution. Our conclusion highlights an underappreciated formation pathway of aromatics-derived HOMs and elucidates detailed formation mechanisms of certain HOMs, which advances our understanding on HOMs and potentially explains the existing gap between model prediction and ambient measurement on the HOMs concentrations.
Kevin J. Nihill, Matthew M. Coggon, Christopher Y. Lim, Abigail R. Koss, Bin Yuan, Jordan E. Krechmer, Kanako Sekimoto, Jose L. Jimenez, Joost de Gouw, Christopher D. Cappa, Colette L. Heald, Carsten Warneke, and Jesse H. Kroll
Atmos. Chem. Phys., 23, 7887–7899, https://doi.org/10.5194/acp-23-7887-2023, https://doi.org/10.5194/acp-23-7887-2023, 2023
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In this work, we collect emissions from controlled burns of biomass fuels that can be found in the western United States into an environmental chamber in order to simulate their oxidation as they pass through the atmosphere. These findings provide a detailed characterization of the composition of the atmosphere downwind of wildfires. In turn, this will help to explore the effects of these changing emissions on downwind populations and will also directly inform atmospheric and climate models.
Caterina Mapelli, James K. Donnelly, Úna E. Hogan, Andrew R. Rickard, Abbie T. Robinson, Fergal Byrne, Con Rob McElroy, Basile F. E. Curchod, Daniel Hollas, and Terry J. Dillon
Atmos. Chem. Phys., 23, 7767–7779, https://doi.org/10.5194/acp-23-7767-2023, https://doi.org/10.5194/acp-23-7767-2023, 2023
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Solvents are chemical compounds with countless uses in the chemical industry, and they also represent one of the main sources of pollution in the chemical sector. Scientists are trying to develop new
greensafer solvents which present favourable advantages when compared to traditional solvents. Since the assessment of these green solvents often lacks air quality considerations, this study aims to understand the behaviour of these compounds, investigating their reactivity in the troposphere.
Roland Benoit, Nesrine Belhadj, Zahraa Dbouk, Maxence Lailliau, and Philippe Dagaut
Atmos. Chem. Phys., 23, 5715–5733, https://doi.org/10.5194/acp-23-5715-2023, https://doi.org/10.5194/acp-23-5715-2023, 2023
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We observed a surprisingly similar set of oxidation product chemical formulas from limonene and α-pinene, including oligomers, formed under cool-flame (present experiments) and simulated atmospheric oxidation (literature). Data analysis indicated that a subset of chemical formulas is common to all experiments independently of experimental conditions. Also, this study indicates that many detected chemical formulas can be ascribed to an autooxidation reaction.
Melissa Meder, Otso Peräkylä, Jonathan G. Varelas, Jingyi Luo, Runlong Cai, Yanjun Zhang, Theo Kurtén, Matthieu Riva, Matti Rissanen, Franz M. Geiger, Regan J. Thomson, and Mikael Ehn
Atmos. Chem. Phys., 23, 4373–4390, https://doi.org/10.5194/acp-23-4373-2023, https://doi.org/10.5194/acp-23-4373-2023, 2023
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We discuss and show the viability of a method where multiple isotopically labelled precursors are used for probing the formation pathways of highly oxygenated organic molecules (HOMs) from the oxidation of the monoterpene a-pinene. HOMs are very important for secondary organic aerosol (SOA) formation in forested regions, and monoterpenes are the single largest source of SOA globally. The fast reactions forming HOMs have thus far remained elusive despite considerable efforts over the last decade.
Philip T. M. Carlsson, Luc Vereecken, Anna Novelli, François Bernard, Steven S. Brown, Bellamy Brownwood, Changmin Cho, John N. Crowley, Patrick Dewald, Peter M. Edwards, Nils Friedrich, Juliane L. Fry, Mattias Hallquist, Luisa Hantschke, Thorsten Hohaus, Sungah Kang, Jonathan Liebmann, Alfred W. Mayhew, Thomas Mentel, David Reimer, Franz Rohrer, Justin Shenolikar, Ralf Tillmann, Epameinondas Tsiligiannis, Rongrong Wu, Andreas Wahner, Astrid Kiendler-Scharr, and Hendrik Fuchs
Atmos. Chem. Phys., 23, 3147–3180, https://doi.org/10.5194/acp-23-3147-2023, https://doi.org/10.5194/acp-23-3147-2023, 2023
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The investigation of the night-time oxidation of the most abundant hydrocarbon, isoprene, in chamber experiments shows the importance of reaction pathways leading to epoxy products, which could enhance particle formation, that have so far not been accounted for. The chemical lifetime of organic nitrates from isoprene is long enough for the majority to be further oxidized the next day by daytime oxidants.
Kevin D. Easterbrook, Mitchell A. Vona, Kiana Nayebi-Astaneh, Amanda M. Miller, and Hans D. Osthoff
Atmos. Chem. Phys., 23, 311–322, https://doi.org/10.5194/acp-23-311-2023, https://doi.org/10.5194/acp-23-311-2023, 2023
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The trace gas peroxypropionyl nitrate (PPN) is generated in photochemical smog, phytotoxic, a strong eye irritant, and possibly mutagenic. Here, its solubility and reactivity in water and in octanol were investigated using a bubble flow apparatus, yielding its Henry's law constant and octanol–water partition coefficient (Kow). The results allow the fate of PPN to be more accurately constrained in atmospheric chemical transport models, including its uptake on clouds, organic aerosol, and leaves.
Qing Ye, Matthew B. Goss, Jordan E. Krechmer, Francesca Majluf, Alexander Zaytsev, Yaowei Li, Joseph R. Roscioli, Manjula Canagaratna, Frank N. Keutsch, Colette L. Heald, and Jesse H. Kroll
Atmos. Chem. Phys., 22, 16003–16015, https://doi.org/10.5194/acp-22-16003-2022, https://doi.org/10.5194/acp-22-16003-2022, 2022
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The atmospheric oxidation of dimethyl sulfide (DMS) is a major natural source of sulfate particles in the atmosphere. However, its mechanism is poorly constrained. In our work, laboratory measurements and mechanistic modeling were conducted to comprehensively investigate DMS oxidation products and key reaction rates. We find that the peroxy radical (RO2) has a controlling effect on product distribution and aerosol yield, with the isomerization of RO2 leading to the suppression of aerosol yield.
Caterina Mapelli, Juliette V. Schleicher, Alex Hawtin, Conor D. Rankine, Fiona C. Whiting, Fergal Byrne, C. Rob McElroy, Claudiu Roman, Cecilia Arsene, Romeo I. Olariu, Iustinian G. Bejan, and Terry J. Dillon
Atmos. Chem. Phys., 22, 14589–14602, https://doi.org/10.5194/acp-22-14589-2022, https://doi.org/10.5194/acp-22-14589-2022, 2022
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Solvents represent an important source of pollution from the chemical industry. New "green" solvents aim to replace toxic solvents with new molecules made from renewable sources and designed to be less harmful. Whilst these new molecules are selected according to toxicity and other characteristics, no consideration has yet been included on air quality. Studying the solvent breakdown in air, we found that TMO has a lower impact on air quality than traditional solvents with similar properties.
Kai Song, Song Guo, Yuanzheng Gong, Daqi Lv, Yuan Zhang, Zichao Wan, Tianyu Li, Wenfei Zhu, Hui Wang, Ying Yu, Rui Tan, Ruizhe Shen, Sihua Lu, Shuangde Li, Yunfa Chen, and Min Hu
Atmos. Chem. Phys., 22, 9827–9841, https://doi.org/10.5194/acp-22-9827-2022, https://doi.org/10.5194/acp-22-9827-2022, 2022
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Emissions from four typical Chinese domestic cooking and fried chicken using four kinds of oils were investigated to illustrate the impact of cooking style and oil. Of the estimated SOA, 10.2 %–32.0 % could be explained by S/IVOC oxidation. Multiway principal component analysis (MPCA) emphasizes the importance of the unsaturated fatty acid-alkadienal volatile product mechanism (oil autoxidation) accelerated by the cooking and heating procedure.
Michelia Dam, Danielle C. Draper, Andrey Marsavin, Juliane L. Fry, and James N. Smith
Atmos. Chem. Phys., 22, 9017–9031, https://doi.org/10.5194/acp-22-9017-2022, https://doi.org/10.5194/acp-22-9017-2022, 2022
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We performed chamber experiments to measure the composition of the gas-phase reaction products of nitrate-radical-initiated oxidation of four monoterpenes. The total organic yield, effective oxygen-to-carbon ratio, and dimer-to-monomer ratio were correlated with the observed particle formation for the monoterpene systems with some exceptions. The Δ-carene system produced the most particles, followed by β-pinene, with the α-pinene and α-thujene systems producing no particles.
Jacky Yat Sing Pang, Anna Novelli, Martin Kaminski, Ismail-Hakki Acir, Birger Bohn, Philip T. M. Carlsson, Changmin Cho, Hans-Peter Dorn, Andreas Hofzumahaus, Xin Li, Anna Lutz, Sascha Nehr, David Reimer, Franz Rohrer, Ralf Tillmann, Robert Wegener, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 22, 8497–8527, https://doi.org/10.5194/acp-22-8497-2022, https://doi.org/10.5194/acp-22-8497-2022, 2022
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This study investigates the radical chemical budget during the limonene oxidation at different atmospheric-relevant NO concentrations in chamber experiments under atmospheric conditions. It is found that the model–measurement discrepancies of HO2 and RO2 are very large at low NO concentrations that are typical for forested environments. Possible additional processes impacting HO2 and RO2 concentrations are discussed.
Carmen Maria Tovar, Ian Barnes, Iustinian Gabriel Bejan, and Peter Wiesen
Atmos. Chem. Phys., 22, 6989–7004, https://doi.org/10.5194/acp-22-6989-2022, https://doi.org/10.5194/acp-22-6989-2022, 2022
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This work explores the kinetics and reactivity of epoxides towards the OH radical using two different simulation chambers. Estimation of the rate coefficients has also been made using different structure–activity relationship (SAR) approaches. The results indicate a direct influence of the structural and geometric properties of the epoxides not considered in SAR estimations, influencing the reactivity of these compounds. The outcomes of this work are in very good agreement with previous studies.
Axel Fouqueau, Manuela Cirtog, Mathieu Cazaunau, Edouard Pangui, Jean-François Doussin, and Bénédicte Picquet-Varrault
Atmos. Chem. Phys., 22, 6411–6434, https://doi.org/10.5194/acp-22-6411-2022, https://doi.org/10.5194/acp-22-6411-2022, 2022
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Biogenic volatile organic compounds are intensely emitted by forests and crops and react with the nitrate radical during the nighttime to form functionalized products. The purpose of this study is to furnish kinetic and mechanistic data for terpinolene and β-caryophyllene, using simulation chamber experiments. Rate constants have been measured using both relative and absolute methods, and mechanistic studies have been conducted in order to identify and quantify the main reaction products.
Yuanyuan Luo, Olga Garmash, Haiyan Li, Frans Graeffe, Arnaud P. Praplan, Anssi Liikanen, Yanjun Zhang, Melissa Meder, Otso Peräkylä, Josep Peñuelas, Ana María Yáñez-Serrano, and Mikael Ehn
Atmos. Chem. Phys., 22, 5619–5637, https://doi.org/10.5194/acp-22-5619-2022, https://doi.org/10.5194/acp-22-5619-2022, 2022
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Diterpenes were only recently observed in the atmosphere, and little is known of their atmospheric fates. We explored the ozonolysis of the diterpene kaurene in a chamber, and we characterized the oxidation products for the first time using chemical ionization mass spectrometry. Our findings highlight similarities and differences between diterpenes and smaller terpenes during their atmospheric oxidation.
Wenyu Sun, Matias Berasategui, Andrea Pozzer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 22, 4969–4984, https://doi.org/10.5194/acp-22-4969-2022, https://doi.org/10.5194/acp-22-4969-2022, 2022
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The reaction between OH and SO2 is a termolecular process that in the atmosphere results in the formation of H2SO4 and thus aerosols. We present the first temperature- and pressure-dependent measurements of the rate coefficients in N2. This is also the first study to examine the effects of water vapour on the kinetics of this reaction. Our results indicate the rate coefficient is larger than that recommended by evaluation panels, with deviations of up to 30 % in some parts of the atmosphere.
Haoyu Jiang, Yingyao He, Yiqun Wang, Sheng Li, Bin Jiang, Luca Carena, Xue Li, Lihua Yang, Tiangang Luan, Davide Vione, and Sasho Gligorovski
Atmos. Chem. Phys., 22, 4237–4252, https://doi.org/10.5194/acp-22-4237-2022, https://doi.org/10.5194/acp-22-4237-2022, 2022
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Heterogeneous oxidation of SO2 is suggested to be one of the most important pathways for sulfate formation during extreme haze events in China, yet the exact mechanism remains highly uncertain. Our study reveals that ubiquitous compounds at the sea surface PAHS and DMSO, when exposed to SO2 under simulated sunlight irradiation, generate abundant organic sulfur compounds, providing implications for air-sea interaction and secondary organic aerosols formation processes.
María Asensio, María Antiñolo, Sergio Blázquez, José Albaladejo, and Elena Jiménez
Atmos. Chem. Phys., 22, 2689–2701, https://doi.org/10.5194/acp-22-2689-2022, https://doi.org/10.5194/acp-22-2689-2022, 2022
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The diurnal atmospheric degradation of 2-methylbutanal, 2 MB, emitted by sources like vegetation or the poultry industry is evaluated in this work. Sunlight and oxidants like hydroxyl (OH) radicals and chlorine (Cl) atoms initiate this degradation. Measurements of how fast 2 MB is degraded and what products are generated are presented. The lifetime of 2 MB is around 1 h at noon, when the OH reaction dominates. Thus, 2 MB will not be transported far, affecting only local air quality.
Claudiu Roman, Cecilia Arsene, Iustinian Gabriel Bejan, and Romeo Iulian Olariu
Atmos. Chem. Phys., 22, 2203–2219, https://doi.org/10.5194/acp-22-2203-2022, https://doi.org/10.5194/acp-22-2203-2022, 2022
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Gas-phase reaction rate coefficients of OH radicals with four nitrocatechols have been investigated for the first time by using ESC-Q-UAIC chamber facilities. The reactivity of all investigated nitrocatechols is influenced by the formation of the intramolecular H-bonds that are connected to the deactivating electromeric effect of the NO2 group. For the 3-nitrocatechol compounds, the electromeric effect of the
freeOH group is diminished by the deactivating E-effect of the NO2 group.
Zhiyuan Gao, Nicolas-Xavier Geilfus, Alfonso Saiz-Lopez, and Feiyue Wang
Atmos. Chem. Phys., 22, 1811–1824, https://doi.org/10.5194/acp-22-1811-2022, https://doi.org/10.5194/acp-22-1811-2022, 2022
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Every spring in the Arctic, a series of photochemical events occur over the ice-covered ocean, known as bromine explosion events, ozone depletion events, and mercury depletion events. Here we report the re-creation of these events at an outdoor sea ice facility in Winnipeg, Canada, far away from the Arctic. The success provides a new platform with new opportunities to uncover fundamental mechanisms of these Arctic springtime phenomena and how they may change in a changing climate.
Haichao Wang, Chao Peng, Xuan Wang, Shengrong Lou, Keding Lu, Guicheng Gan, Xiaohong Jia, Xiaorui Chen, Jun Chen, Hongli Wang, Shaojia Fan, Xinming Wang, and Mingjin Tang
Atmos. Chem. Phys., 22, 1845–1859, https://doi.org/10.5194/acp-22-1845-2022, https://doi.org/10.5194/acp-22-1845-2022, 2022
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Via combining laboratory and modeling work, we found that heterogeneous reaction of N2O5 with saline mineral dust aerosol could be an important source of tropospheric ClNO2 in inland regions.
Mike J. Newland, Yangang Ren, Max R. McGillen, Lisa Michelat, Véronique Daële, and Abdelwahid Mellouki
Atmos. Chem. Phys., 22, 1761–1772, https://doi.org/10.5194/acp-22-1761-2022, https://doi.org/10.5194/acp-22-1761-2022, 2022
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Wildfires are increasing in extent and severity, driven by climate change. Such fires emit large amounts of volatile organic compounds (VOCs) to the atmosphere. Many of these, such as the furans studied here, are very reactive and are rapidly converted to other VOCs, which are expected to have negative health effects and to further impact the climate. Here, we establish the importance of the nitrate radical for removing these compounds both during the night and during the day.
Delaney B. Kilgour, Gordon A. Novak, Jon S. Sauer, Alexia N. Moore, Julie Dinasquet, Sarah Amiri, Emily B. Franklin, Kathryn Mayer, Margaux Winter, Clare K. Morris, Tyler Price, Francesca Malfatti, Daniel R. Crocker, Christopher Lee, Christopher D. Cappa, Allen H. Goldstein, Kimberly A. Prather, and Timothy H. Bertram
Atmos. Chem. Phys., 22, 1601–1613, https://doi.org/10.5194/acp-22-1601-2022, https://doi.org/10.5194/acp-22-1601-2022, 2022
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We report measurements of gas-phase volatile organosulfur molecules made during a mesocosm phytoplankton bloom experiment. Dimethyl sulfide (DMS), methanethiol (MeSH), and benzothiazole accounted for on average over 90 % of total gas-phase sulfur emissions. This work focuses on factors controlling the production and emission of DMS and MeSH and the role of non-DMS molecules (such as MeSH and benzothiazole) in secondary sulfate formation in coastal marine environments.
Niklas Illmann, Iulia Patroescu-Klotz, and Peter Wiesen
Atmos. Chem. Phys., 21, 18557–18572, https://doi.org/10.5194/acp-21-18557-2021, https://doi.org/10.5194/acp-21-18557-2021, 2021
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Understanding the chemistry of biomass burning plumes is of global interest. Within this work we investigated the OH radical reaction of 3-penten-2-one, which has been identified in biomass burning emissions. We observed the primary formation of peroxyacetyl nitrate (PAN), a key NOx reservoir species. Besides, PAN precursors were also identified as main oxidation products. 3-Penten-2-one is shown to be an example explaining rapid PAN formation within young biomass burning plumes.
Zhaofeng Tan, Luisa Hantschke, Martin Kaminski, Ismail-Hakki Acir, Birger Bohn, Changmin Cho, Hans-Peter Dorn, Xin Li, Anna Novelli, Sascha Nehr, Franz Rohrer, Ralf Tillmann, Robert Wegener, Andreas Hofzumahaus, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 21, 16067–16091, https://doi.org/10.5194/acp-21-16067-2021, https://doi.org/10.5194/acp-21-16067-2021, 2021
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The photo-oxidation of myrcene, a monoterpene species emitted by plants, was investigated at atmospheric conditions in the outdoor simulation chamber SAPHIR. The chemical structure of myrcene is partly similar to isoprene. Therefore, it can be expected that hydrogen shift reactions could play a role as observed for isoprene. In this work, their potential impact on the regeneration efficiency of hydroxyl radicals is investigated.
Shijie Yu, Fangcheng Su, Shasha Yin, Shenbo Wang, Ruixin Xu, Bing He, Xiangge Fan, Minghao Yuan, and Ruiqin Zhang
Atmos. Chem. Phys., 21, 15239–15257, https://doi.org/10.5194/acp-21-15239-2021, https://doi.org/10.5194/acp-21-15239-2021, 2021
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This study measured 106 VOC species using a GC-MS/FID. Meanwhile, the WRF-CMAQ model was used to investigate the nonlinearity of the O3 response to precursor reductions. This study highlights the effectiveness of stringent emission controls in relation to solvent utilization and coal combustion. However, unreasonable emission reduction may aggravate ozone pollution during control periods. It is suggested that emission-reduction ratios of the precursors (VOC : NOx) should be more than 2.
Niklas Illmann, Rodrigo Gastón Gibilisco, Iustinian Gabriel Bejan, Iulia Patroescu-Klotz, and Peter Wiesen
Atmos. Chem. Phys., 21, 13667–13686, https://doi.org/10.5194/acp-21-13667-2021, https://doi.org/10.5194/acp-21-13667-2021, 2021
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Within this work we determined the rate coefficients and products of the reaction of unsaturated ketones with OH radicals in an effort to complete the gaps in the knowledge needed for modelling chemistry in the atmosphere. Both substances are potentially emitted by biomass burning, industrial activities or formed in the troposphere by oxidation of terpenes. As products we identified aldehydes and ketones which in turn are known to be responsible for the transportation of NOx species.
Yangang Ren, Li Zhou, Abdelwahid Mellouki, Véronique Daële, Mahmoud Idir, Steven S. Brown, Branko Ruscic, Robert S. Paton, Max R. McGillen, and A. R. Ravishankara
Atmos. Chem. Phys., 21, 13537–13551, https://doi.org/10.5194/acp-21-13537-2021, https://doi.org/10.5194/acp-21-13537-2021, 2021
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Aromatic aldehydes are a family of compounds emitted into the atmosphere from both anthropogenic and biogenic sources that are formed from the degradation of aromatic hydrocarbons. Their atmospheric degradation may impact air quality. We report on their atmospheric degradation through reaction with NO3, which is useful to estimate their atmospheric lifetimes. We have also attempted to elucidate the mechanism of these reactions via studies of isotopic substitution and quantum chemistry.
Luisa Hantschke, Anna Novelli, Birger Bohn, Changmin Cho, David Reimer, Franz Rohrer, Ralf Tillmann, Marvin Glowania, Andreas Hofzumahaus, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 21, 12665–12685, https://doi.org/10.5194/acp-21-12665-2021, https://doi.org/10.5194/acp-21-12665-2021, 2021
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The reactions of Δ3-carene with ozone and the hydroxyl radical (OH) and the photolysis and OH reaction of caronaldehyde were investigated in the simulation chamber SAPHIR. Reaction rate constants of these reactions were determined. Caronaldehyde yields of the ozonolysis and OH reaction were determined. The organic nitrate yield of the reaction of Δ3-carene and caronaldehyde-derived peroxy radicals with NO was determined. The ROx budget (ROx = OH+HO2+RO2) was also investigated.
Letizia Abis, Carmen Kalalian, Bastien Lunardelli, Tao Wang, Liwu Zhang, Jianmin Chen, Sébastien Perrier, Benjamin Loubet, Raluca Ciuraru, and Christian George
Atmos. Chem. Phys., 21, 12613–12629, https://doi.org/10.5194/acp-21-12613-2021, https://doi.org/10.5194/acp-21-12613-2021, 2021
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Biogenic volatile organic compound (BVOC) emissions from rapeseed leaf litter have been investigated by means of a controlled atmospheric simulation chamber. The diversity of emitted VOCs increased also in the presence of UV light irradiation. SOA formation was observed when leaf litter was exposed to both UV light and ozone, indicating a potential contribution to particle formation or growth at local scales.
Xi Cheng, Qi Chen, Yong Jie Li, Yan Zheng, Keren Liao, and Guancong Huang
Atmos. Chem. Phys., 21, 12005–12019, https://doi.org/10.5194/acp-21-12005-2021, https://doi.org/10.5194/acp-21-12005-2021, 2021
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In this study, we conducted laboratory studies to investigate the formation of gas-phase highly oxygenated organic molecules (HOMs). We provide a thorough analysis on the importance of multistep auto-oxidation and multigeneration OH reactions. We also give an intensive investigation on the roles of high-NO2 conditions that represent a wide range of anthropogenically influenced environments.
Rongrong Wu, Luc Vereecken, Epameinondas Tsiligiannis, Sungah Kang, Sascha R. Albrecht, Luisa Hantschke, Defeng Zhao, Anna Novelli, Hendrik Fuchs, Ralf Tillmann, Thorsten Hohaus, Philip T. M. Carlsson, Justin Shenolikar, François Bernard, John N. Crowley, Juliane L. Fry, Bellamy Brownwood, Joel A. Thornton, Steven S. Brown, Astrid Kiendler-Scharr, Andreas Wahner, Mattias Hallquist, and Thomas F. Mentel
Atmos. Chem. Phys., 21, 10799–10824, https://doi.org/10.5194/acp-21-10799-2021, https://doi.org/10.5194/acp-21-10799-2021, 2021
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Isoprene is the biogenic volatile organic compound with the largest emissions rates. The nighttime reaction of isoprene with the NO3 radical has a large potential to contribute to SOA. We classified isoprene nitrates into generations and proposed formation pathways. Considering the potential functionalization of the isoprene nitrates we propose that mainly isoprene dimers contribute to SOA formation from the isoprene NO3 reactions with at least a 5 % mass yield.
Defeng Zhao, Iida Pullinen, Hendrik Fuchs, Stephanie Schrade, Rongrong Wu, Ismail-Hakki Acir, Ralf Tillmann, Franz Rohrer, Jürgen Wildt, Yindong Guo, Astrid Kiendler-Scharr, Andreas Wahner, Sungah Kang, Luc Vereecken, and Thomas F. Mentel
Atmos. Chem. Phys., 21, 9681–9704, https://doi.org/10.5194/acp-21-9681-2021, https://doi.org/10.5194/acp-21-9681-2021, 2021
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The reaction of isoprene, a biogenic volatile organic compound with the globally largest emission rates, with NO3, an nighttime oxidant influenced heavily by anthropogenic emissions, forms a large number of highly oxygenated organic molecules (HOM). These HOM are formed via one or multiple oxidation steps, followed by autoxidation. Their total yield is much higher than that in the daytime oxidation of isoprene. They may play an important role in nighttime organic aerosol formation and growth.
Chelsea E. Stockwell, Matthew M. Coggon, Georgios I. Gkatzelis, John Ortega, Brian C. McDonald, Jeff Peischl, Kenneth Aikin, Jessica B. Gilman, Michael Trainer, and Carsten Warneke
Atmos. Chem. Phys., 21, 6005–6022, https://doi.org/10.5194/acp-21-6005-2021, https://doi.org/10.5194/acp-21-6005-2021, 2021
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Volatile chemical products are emerging as a large source of petrochemical organics in urban environments. We identify markers for the coatings category by linking ambient observations to laboratory measurements, investigating volatile organic compound (VOC) composition, and quantifying key VOC emissions via controlled evaporation experiments. Ingredients and sales surveys are used to confirm the prevalence and usage trends to support the assignment of water and solvent-borne coating tracers.
Abdelwahid Mellouki, Markus Ammann, R. Anthony Cox, John N. Crowley, Hartmut Herrmann, Michael E. Jenkin, V. Faye McNeill, Jürgen Troe, and Timothy J. Wallington
Atmos. Chem. Phys., 21, 4797–4808, https://doi.org/10.5194/acp-21-4797-2021, https://doi.org/10.5194/acp-21-4797-2021, 2021
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Volatile organic compounds play an important role in atmospheric chemistry. This article, the eighth in the series, presents kinetic and photochemical data sheets evaluated by the IUPAC Task Group on Atmospheric Chemical Kinetic Data Evaluation. It covers the gas-phase reactions of organic species with four, or more, carbon atoms (≥ C4) including thermal reactions of closed-shell organic species with HO and NO3 radicals and their photolysis. These data are important for atmospheric models.
Michael Priestley, Thomas J. Bannan, Michael Le Breton, Stephen D. Worrall, Sungah Kang, Iida Pullinen, Sebastian Schmitt, Ralf Tillmann, Einhard Kleist, Defeng Zhao, Jürgen Wildt, Olga Garmash, Archit Mehra, Asan Bacak, Dudley E. Shallcross, Astrid Kiendler-Scharr, Åsa M. Hallquist, Mikael Ehn, Hugh Coe, Carl J. Percival, Mattias Hallquist, Thomas F. Mentel, and Gordon McFiggans
Atmos. Chem. Phys., 21, 3473–3490, https://doi.org/10.5194/acp-21-3473-2021, https://doi.org/10.5194/acp-21-3473-2021, 2021
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A significant fraction of emissions from human activity consists of aromatic hydrocarbons, e.g. benzene, which oxidise to form new compounds important for particle growth. Characterisation of benzene oxidation products highlights the range of species produced as well as their chemical properties and contextualises them within relevant frameworks, e.g. MCM. Cluster analysis of the oxidation product time series distinguishes behaviours of CHON compounds that could aid in identifying functionality.
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Short summary
Landscape fires are a major source of greenhouse gases and aerosols, particularly in sub-tropical savannas. Stable carbon isotopes in emissions can be used to trace the contribution of C3 plants (e.g. trees or shrubs) and C4 plants (e.g. savanna grasses) to greenhouse gases and aerosols if the process is well understood. This helps us to link individual vegetation types to emissions, identify biomass burning emissions in the atmosphere, and improve the reconstruction of historic fire regimes.
Landscape fires are a major source of greenhouse gases and aerosols, particularly in...
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