Articles | Volume 19, issue 13
https://doi.org/10.5194/acp-19-8687-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Special issue:
https://doi.org/10.5194/acp-19-8687-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Atmospheric measurements of the terrestrial O2 : CO2 exchange ratio of a midlatitude forest
Mark O. Battle
CORRESPONDING AUTHOR
Dept. of Physics & Astronomy, Bowdoin College, Brunswick, ME 04011-8488, USA
J. William Munger
School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138, USA
Margaret Conley
Dept. of Physics & Astronomy, Bowdoin College, Brunswick, ME 04011-8488, USA
Eric Sofen
Dept. of Physics & Astronomy, Bowdoin College, Brunswick, ME 04011-8488, USA
Rebecca Perry
Dept. of Physics & Astronomy, Bowdoin College, Brunswick, ME 04011-8488, USA
Ryan Hart
Dept. of Physics & Astronomy, Bowdoin College, Brunswick, ME 04011-8488, USA
Zane Davis
Dept. of Physics & Astronomy, Bowdoin College, Brunswick, ME 04011-8488, USA
Jacob Scheckman
Dept. of Physics & Astronomy, Bowdoin College, Brunswick, ME 04011-8488, USA
Jayme Woogerd
Dept. of Physics & Astronomy, Bowdoin College, Brunswick, ME 04011-8488, USA
Karina Graeter
Dept. of Physics & Astronomy, Bowdoin College, Brunswick, ME 04011-8488, USA
Samuel Seekins
Dept. of Physics & Astronomy, Bowdoin College, Brunswick, ME 04011-8488, USA
Sasha David
Dept. of Physics & Astronomy, Bowdoin College, Brunswick, ME 04011-8488, USA
John Carpenter
Dept. of Physics & Astronomy, Bowdoin College, Brunswick, ME 04011-8488, USA
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Mark O. Battle, Raine Raynor, Stephen Kesler, and Ralph Keeling
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-765, https://doi.org/10.5194/acp-2022-765, 2023
Preprint withdrawn
Short summary
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For decades, we have used measurements of atmospheric oxygen to understand how much carbon dioxide leaves the atmosphere and enters the land biosphere and the oceans. Until now, these calculations have ignored the release of oxygen associated with the refining of iron, aluminum and copper from their ores. In this article, we show that this release of oxygen is indeed much smaller than all of the other terms that have been included in the calculations and the earlier calculations are valid.
Cathy M. Trudinger, Paul J. Fraser, David M. Etheridge, William T. Sturges, Martin K. Vollmer, Matt Rigby, Patricia Martinerie, Jens Mühle, David R. Worton, Paul B. Krummel, L. Paul Steele, Benjamin R. Miller, Johannes Laube, Francis S. Mani, Peter J. Rayner, Christina M. Harth, Emmanuel Witrant, Thomas Blunier, Jakob Schwander, Simon O'Doherty, and Mark Battle
Atmos. Chem. Phys., 16, 11733–11754, https://doi.org/10.5194/acp-16-11733-2016, https://doi.org/10.5194/acp-16-11733-2016, 2016
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Perfluorocarbons (PFCs) are potent, long-lived and mostly man-made greenhouse gases released to the atmosphere mainly during aluminium production and semiconductor manufacture. Here we present the first continuous histories of three PFCs from 1800 to 2014, derived from measurements of these PFCs in the atmosphere and in air bubbles in polar ice. The records show how human actions have affected these important greenhouse gases over the past century.
V. V. Petrenko, P. Martinerie, P. Novelli, D. M. Etheridge, I. Levin, Z. Wang, T. Blunier, J. Chappellaz, J. Kaiser, P. Lang, L. P. Steele, S. Hammer, J. Mak, R. L. Langenfelds, J. Schwander, J. P. Severinghaus, E. Witrant, G. Petron, M. O. Battle, G. Forster, W. T. Sturges, J.-F. Lamarque, K. Steffen, and J. W. C. White
Atmos. Chem. Phys., 13, 7567–7585, https://doi.org/10.5194/acp-13-7567-2013, https://doi.org/10.5194/acp-13-7567-2013, 2013
Olivia E. Clifton, Donna Schwede, Christian Hogrefe, Jesse O. Bash, Sam Bland, Philip Cheung, Mhairi Coyle, Lisa Emberson, Johannes Flemming, Erick Fredj, Stefano Galmarini, Laurens Ganzeveld, Orestis Gazetas, Ignacio Goded, Christopher D. Holmes, László Horváth, Vincent Huijnen, Qian Li, Paul A. Makar, Ivan Mammarella, Giovanni Manca, J. William Munger, Juan L. Pérez-Camanyo, Jonathan Pleim, Limei Ran, Roberto San Jose, Sam J. Silva, Ralf Staebler, Shihan Sun, Amos P. K. Tai, Eran Tas, Timo Vesala, Tamás Weidinger, Zhiyong Wu, and Leiming Zhang
Atmos. Chem. Phys., 23, 9911–9961, https://doi.org/10.5194/acp-23-9911-2023, https://doi.org/10.5194/acp-23-9911-2023, 2023
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A primary sink of air pollutants is dry deposition. Dry deposition estimates differ across the models used to simulate atmospheric chemistry. Here, we introduce an effort to examine dry deposition schemes from atmospheric chemistry models. We provide our approach’s rationale, document the schemes, and describe datasets used to drive and evaluate the schemes. We also launch the analysis of results by evaluating against observations and identifying the processes leading to model–model differences.
Mark O. Battle, Raine Raynor, Stephen Kesler, and Ralph Keeling
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-765, https://doi.org/10.5194/acp-2022-765, 2023
Preprint withdrawn
Short summary
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For decades, we have used measurements of atmospheric oxygen to understand how much carbon dioxide leaves the atmosphere and enters the land biosphere and the oceans. Until now, these calculations have ignored the release of oxygen associated with the refining of iron, aluminum and copper from their ores. In this article, we show that this release of oxygen is indeed much smaller than all of the other terms that have been included in the calculations and the earlier calculations are valid.
Luke D. Schiferl, Jennifer D. Watts, Erik J. L. Larson, Kyle A. Arndt, Sébastien C. Biraud, Eugénie S. Euskirchen, Jordan P. Goodrich, John M. Henderson, Aram Kalhori, Kathryn McKain, Marikate E. Mountain, J. William Munger, Walter C. Oechel, Colm Sweeney, Yonghong Yi, Donatella Zona, and Róisín Commane
Biogeosciences, 19, 5953–5972, https://doi.org/10.5194/bg-19-5953-2022, https://doi.org/10.5194/bg-19-5953-2022, 2022
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As the Arctic rapidly warms, vast stores of thawing permafrost could release carbon dioxide (CO2) into the atmosphere. We combined observations of atmospheric CO2 concentrations from aircraft and a tower with observed CO2 fluxes from tundra ecosystems and found that the Alaskan North Slope in not a consistent source nor sink of CO2. Our study shows the importance of using both site-level and atmospheric measurements to constrain regional net CO2 fluxes and improve biogenic processes in models.
Archana Dayalu, J. William Munger, Yuxuan Wang, Steven C. Wofsy, Yu Zhao, Thomas Nehrkorn, Chris Nielsen, Michael B. McElroy, and Rachel Chang
Atmos. Chem. Phys., 20, 3569–3588, https://doi.org/10.5194/acp-20-3569-2020, https://doi.org/10.5194/acp-20-3569-2020, 2020
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China has pledged to reduce carbon dioxide emissions per unit GDP by 60–65 % relative to 2005 levels, and to peak carbon emissions overall by 2030. Disagreement among available inventories of Chinese emissions makes it difficult for China to track progress toward its goals and evaluate the efficacy of regional control measures. This study uses a unique set of historical atmospheric observations for the key period from 2005 to 2009 to independently evaluate three different CO2 emission estimates.
Shaojie Song, Meng Gao, Weiqi Xu, Yele Sun, Douglas R. Worsnop, John T. Jayne, Yuzhong Zhang, Lei Zhu, Mei Li, Zhen Zhou, Chunlei Cheng, Yibing Lv, Ying Wang, Wei Peng, Xiaobin Xu, Nan Lin, Yuxuan Wang, Shuxiao Wang, J. William Munger, Daniel J. Jacob, and Michael B. McElroy
Atmos. Chem. Phys., 19, 1357–1371, https://doi.org/10.5194/acp-19-1357-2019, https://doi.org/10.5194/acp-19-1357-2019, 2019
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Chemistry responsible for sulfate production in northern China winter haze remains mysterious. We propose a potentially key pathway through the reaction of formaldehyde and sulfur dioxide that has not been accounted for in previous studies. The special atmospheric conditions favor the formation and existence of their complex, hydroxymethanesulfonate (HMS).
Archana Dayalu, J. William Munger, Steven C. Wofsy, Yuxuan Wang, Thomas Nehrkorn, Yu Zhao, Michael B. McElroy, Chris P. Nielsen, and Kristina Luus
Biogeosciences, 15, 6713–6729, https://doi.org/10.5194/bg-15-6713-2018, https://doi.org/10.5194/bg-15-6713-2018, 2018
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Accounting for the vegetation signal is critical for comprehensive CO2 budget assessment in China. We model and evaluate hourly vegetation carbon dioxide (CO2) exchange (mass per unit area per unit time) in northern China from 2005 to 2009. The model is driven by satellite and meteorological data, is linked to ground-level ecosystem observations, and is applicable to other time periods. We find vegetation uptake of CO2 in summer is comparable to emissions from fossil fuels in northern China.
Archana Dayalu, J. William Munger, Yuxuan Wang, Steven C. Wofsy, Yu Zhao, Thomas Nehrkorn, Chris Nielsen, Michael B. McElroy, and Rachel Chang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-632, https://doi.org/10.5194/acp-2018-632, 2018
Revised manuscript not accepted
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China has pledged reduction of carbon dioxide emissions per unit GDP by 60–65 % relative to 2005 levels, and to peak carbon emissions overall by 2030. Disagreement among available inventories of Chinese emissions makes it difficult for China to track progress toward its goals and evaluate the efficacy of regional control measures. This study uses a unique set of historical atmospheric observations for the key period from 2005–2009 to independently evaluate three different CO2 emissions estimates.
Jason A. Ducker, Christopher D. Holmes, Trevor F. Keenan, Silvano Fares, Allen H. Goldstein, Ivan Mammarella, J. William Munger, and Jordan Schnell
Biogeosciences, 15, 5395–5413, https://doi.org/10.5194/bg-15-5395-2018, https://doi.org/10.5194/bg-15-5395-2018, 2018
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We have developed an accurate method (SynFlux) to estimate ozone deposition and stomatal uptake across 103 flux tower sites (43 US, 60 Europe), where ozone concentrations and fluxes have not been measured. In all, the SynFlux public dataset provides monthly values of ozone dry deposition for 926 site years across a wide array of ecosystems. The SynFlux dataset will promote further applications to ecosystem, air quality, or climate modeling across the geoscience community.
Matthew N. Hayek, Marcos Longo, Jin Wu, Marielle N. Smith, Natalia Restrepo-Coupe, Raphael Tapajós, Rodrigo da Silva, David R. Fitzjarrald, Plinio B. Camargo, Lucy R. Hutyra, Luciana F. Alves, Bruce Daube, J. William Munger, Kenia T. Wiedemann, Scott R. Saleska, and Steven C. Wofsy
Biogeosciences, 15, 4833–4848, https://doi.org/10.5194/bg-15-4833-2018, https://doi.org/10.5194/bg-15-4833-2018, 2018
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We investigated the roles that weather and forest disturbances like drought play in shaping changes in ecosystem photosynthesis and carbon exchange in an Amazon forest. We discovered that weather largely influenced differences between years, but a prior drought, which occurred 3 years before measurements started, likely hampered photosynthesis in the first year. This is the first atmospheric evidence that drought can have legacy impacts on Amazon forest photosynthesis.
Dan Lu, Daniel Ricciuto, Anthony Walker, Cosmin Safta, and William Munger
Biogeosciences, 14, 4295–4314, https://doi.org/10.5194/bg-14-4295-2017, https://doi.org/10.5194/bg-14-4295-2017, 2017
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Calibration of terrestrial ecosystem models (TEMs) is important but challenging. This study applies an advanced sampling technique for parameter estimation of a TEM. The results improve the model fit and predictive performance.
Richard Wehr, Róisín Commane, J. William Munger, J. Barry McManus, David D. Nelson, Mark S. Zahniser, Scott R. Saleska, and Steven C. Wofsy
Biogeosciences, 14, 389–401, https://doi.org/10.5194/bg-14-389-2017, https://doi.org/10.5194/bg-14-389-2017, 2017
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Leaf stomata influence both photosynthesis and transpiration, coupling the carbon and water cycles, but there is no direct method for estimating stomatal behavior on the ecosystem scale. We use the ecosystem–atmosphere exchange of water, heat, and carbonyl sulfide to estimate canopy-integrated stomatal conductance by two independent methods. We then use that conductance to show that the seasonal dynamics of transpiration and evaporation are different than represented in current biosphere models.
Kirsti Ashworth, Serena H. Chung, Karena A. McKinney, Ying Liu, J. William Munger, Scot T. Martin, and Allison L. Steiner
Atmos. Chem. Phys., 16, 15461–15484, https://doi.org/10.5194/acp-16-15461-2016, https://doi.org/10.5194/acp-16-15461-2016, 2016
Kaniska Mallick, Ivonne Trebs, Eva Boegh, Laura Giustarini, Martin Schlerf, Darren T. Drewry, Lucien Hoffmann, Celso von Randow, Bart Kruijt, Alessandro Araùjo, Scott Saleska, James R. Ehleringer, Tomas F. Domingues, Jean Pierre H. B. Ometto, Antonio D. Nobre, Osvaldo Luiz Leal de Moraes, Matthew Hayek, J. William Munger, and Steven C. Wofsy
Hydrol. Earth Syst. Sci., 20, 4237–4264, https://doi.org/10.5194/hess-20-4237-2016, https://doi.org/10.5194/hess-20-4237-2016, 2016
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While quantifying vegetation water use over multiple plant function types in the Amazon Basin, we found substantial biophysical control during drought as well as a water-stress period and dominant climatic control during a water surplus period. This work has direct implication in understanding the resilience of the Amazon forest in the spectre of frequent drought menace as well as the role of drought-induced plant biophysical functioning in modulating the water-carbon coupling in this ecosystem.
Cathy M. Trudinger, Paul J. Fraser, David M. Etheridge, William T. Sturges, Martin K. Vollmer, Matt Rigby, Patricia Martinerie, Jens Mühle, David R. Worton, Paul B. Krummel, L. Paul Steele, Benjamin R. Miller, Johannes Laube, Francis S. Mani, Peter J. Rayner, Christina M. Harth, Emmanuel Witrant, Thomas Blunier, Jakob Schwander, Simon O'Doherty, and Mark Battle
Atmos. Chem. Phys., 16, 11733–11754, https://doi.org/10.5194/acp-16-11733-2016, https://doi.org/10.5194/acp-16-11733-2016, 2016
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Perfluorocarbons (PFCs) are potent, long-lived and mostly man-made greenhouse gases released to the atmosphere mainly during aluminium production and semiconductor manufacture. Here we present the first continuous histories of three PFCs from 1800 to 2014, derived from measurements of these PFCs in the atmosphere and in air bubbles in polar ice. The records show how human actions have affected these important greenhouse gases over the past century.
Dene R. Bowdalo, Mathew J. Evans, and Eric D. Sofen
Atmos. Chem. Phys., 16, 8295–8308, https://doi.org/10.5194/acp-16-8295-2016, https://doi.org/10.5194/acp-16-8295-2016, 2016
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We introduce a new methodology for the assessment of atmospheric models with observations. We apply a spectral analysis methodology to hourly ozone observations and the equivalent model output. The spectrally transformed observational data show significant peaks on daily and annual timescales. Comparison between the amplitude and phase of these peaks introduces a new comparison methodology between model and measurements. We find the model shows significant biases on an annual timescale.
Maria Zatko, Lei Geng, Becky Alexander, Eric Sofen, and Katarina Klein
Atmos. Chem. Phys., 16, 2819–2842, https://doi.org/10.5194/acp-16-2819-2016, https://doi.org/10.5194/acp-16-2819-2016, 2016
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We have incorporated an idealized snowpack with a nitrate photolysis parameterization into a global chemical transport model (GEOS-Chem) to examine the implications of snow nitrate photolysis for boundary layer chemistry, the recycling and redistribution of reactive nitrogen, and the preservation of ice-core nitrate in ice cores across Antarctica and Greenland. We also examine the sensitivity of these processes to meteorological parameters and chemical, optical, and physical snow properties.
E. D. Sofen, D. Bowdalo, M. J. Evans, F. Apadula, P. Bonasoni, M. Cupeiro, R. Ellul, I. E. Galbally, R. Girgzdiene, S. Luppo, M. Mimouni, A. C. Nahas, M. Saliba, and K. Tørseth
Earth Syst. Sci. Data, 8, 41–59, https://doi.org/10.5194/essd-8-41-2016, https://doi.org/10.5194/essd-8-41-2016, 2016
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We have brought together all publicly available surface ozone observations from online databases from 1971–2015, with 2200 sites representing regional background conditions appropriate for the evaluation of chemical transport and chemistry-climate models for projects such as the Chemistry-Climate Model Initiative. Gridded data sets of ozone metrics (mean, percentiles, MDA8, SOMO35, etc.) are available from the British Atmospheric Data Centre.
E. D. Sofen, D. Bowdalo, and M. J. Evans
Atmos. Chem. Phys., 16, 1445–1457, https://doi.org/10.5194/acp-16-1445-2016, https://doi.org/10.5194/acp-16-1445-2016, 2016
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We explore the global representativeness of a global surface ozone data set from a range of perspectives (area, biomes, chemical regimes, model uncertainty, model trends). We conclude that the current network fails to provide sufficient constraints for important regions/regimes, leading to uncertainty for a range of atmospheric composition challenges. We suggest 20 new locations for making surface ozone observations, which would significantly enhance our observational capability.
E. D. Sofen, M. J. Evans, and A. C. Lewis
Atmos. Chem. Phys., 15, 13627–13632, https://doi.org/10.5194/acp-15-13627-2015, https://doi.org/10.5194/acp-15-13627-2015, 2015
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As an air pollutant, O3 is monitored photometrically to assess compliance with air quality legislation. A recent study found a 1.8% reduction in its absorption cross section, which would lead to an equivalent increase in observed O3 concentrations. We estimate this would increase the number of sites out of compliance with air quality regulations in the EU and US by 20%. We draw attention to how small changes in gas metrology impacts attainment and compliance with legal air quality standards.
L. Molina, G. Broquet, P. Imbach, F. Chevallier, B. Poulter, D. Bonal, B. Burban, M. Ramonet, L. V. Gatti, S. C. Wofsy, J. W. Munger, E. Dlugokencky, and P. Ciais
Atmos. Chem. Phys., 15, 8423–8438, https://doi.org/10.5194/acp-15-8423-2015, https://doi.org/10.5194/acp-15-8423-2015, 2015
Z. Y. Wu, L. Zhang, X. M. Wang, and J. W. Munger
Atmos. Chem. Phys., 15, 7487–7496, https://doi.org/10.5194/acp-15-7487-2015, https://doi.org/10.5194/acp-15-7487-2015, 2015
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In this study, we have developed a modified micrometeorological gradient method (MGM), although based on existing micrometeorological theory, to estimate O3 dry deposition fluxes over a forest canopy using concentration gradients between a level above and a level below the canopy top. The new method provides an alternative approach in monitoring/estimating long-term deposition fluxes of similar pollutants over tall canopies and is expected to be useful for the scientific community.
G. Wohlfahrt, C. Amelynck, C. Ammann, A. Arneth, I. Bamberger, A. H. Goldstein, L. Gu, A. Guenther, A. Hansel, B. Heinesch, T. Holst, L. Hörtnagl, T. Karl, Q. Laffineur, A. Neftel, K. McKinney, J. W. Munger, S. G. Pallardy, G. W. Schade, R. Seco, and N. Schoon
Atmos. Chem. Phys., 15, 7413–7427, https://doi.org/10.5194/acp-15-7413-2015, https://doi.org/10.5194/acp-15-7413-2015, 2015
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Methanol is the second most abundant volatile organic compound in the troposphere and plays a significant role in atmospheric chemistry. While there is consensus about the dominant role of plants as the major source and the reaction with OH as the major sink, global methanol budgets diverge considerably in terms of source/sink estimates. Here we present micrometeorological methanol flux data from eight sites in order to provide a first cross-site synthesis of the terrestrial methanol exchange.
L. K. Meredith, R. Commane, J. W. Munger, A. Dunn, J. Tang, S. C. Wofsy, and R. G. Prinn
Atmos. Meas. Tech., 7, 2787–2805, https://doi.org/10.5194/amt-7-2787-2014, https://doi.org/10.5194/amt-7-2787-2014, 2014
E. D. Sofen, B. Alexander, E. J. Steig, M. H. Thiemens, S. A. Kunasek, H. M. Amos, A. J. Schauer, M. G. Hastings, J. Bautista, T. L. Jackson, L. E. Vogel, J. R. McConnell, D. R. Pasteris, and E. S. Saltzman
Atmos. Chem. Phys., 14, 5749–5769, https://doi.org/10.5194/acp-14-5749-2014, https://doi.org/10.5194/acp-14-5749-2014, 2014
A. E. Andrews, J. D. Kofler, M. E. Trudeau, J. C. Williams, D. H. Neff, K. A. Masarie, D. Y. Chao, D. R. Kitzis, P. C. Novelli, C. L. Zhao, E. J. Dlugokencky, P. M. Lang, M. J. Crotwell, M. L. Fischer, M. J. Parker, J. T. Lee, D. D. Baumann, A. R. Desai, C. O. Stanier, S. F. J. De Wekker, D. E. Wolfe, J. W. Munger, and P. P. Tans
Atmos. Meas. Tech., 7, 647–687, https://doi.org/10.5194/amt-7-647-2014, https://doi.org/10.5194/amt-7-647-2014, 2014
P. C. Stoy, M. C. Dietze, A. D. Richardson, R. Vargas, A. G. Barr, R. S. Anderson, M. A. Arain, I. T. Baker, T. A. Black, J. M. Chen, R. B. Cook, C. M. Gough, R. F. Grant, D. Y. Hollinger, R. C. Izaurralde, C. J. Kucharik, P. Lafleur, B. E. Law, S. Liu, E. Lokupitiya, Y. Luo, J. W. Munger, C. Peng, B. Poulter, D. T. Price, D. M. Ricciuto, W. J. Riley, A. K. Sahoo, K. Schaefer, C. R. Schwalm, H. Tian, H. Verbeeck, and E. Weng
Biogeosciences, 10, 6893–6909, https://doi.org/10.5194/bg-10-6893-2013, https://doi.org/10.5194/bg-10-6893-2013, 2013
V. V. Petrenko, P. Martinerie, P. Novelli, D. M. Etheridge, I. Levin, Z. Wang, T. Blunier, J. Chappellaz, J. Kaiser, P. Lang, L. P. Steele, S. Hammer, J. Mak, R. L. Langenfelds, J. Schwander, J. P. Severinghaus, E. Witrant, G. Petron, M. O. Battle, G. Forster, W. T. Sturges, J.-F. Lamarque, K. Steffen, and J. W. C. White
Atmos. Chem. Phys., 13, 7567–7585, https://doi.org/10.5194/acp-13-7567-2013, https://doi.org/10.5194/acp-13-7567-2013, 2013
Related subject area
Subject: Gases | Research Activity: Field Measurements | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
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Intensive photochemical oxidation in the marine atmosphere: Evidence from direct radical measurements
Measurement Report: The Palau Atmospheric Observatory and its Ozonesonde Record - Continuous Monitoring of Tropospheric Composition and Dynamics in the Tropical West Pacific
Shigeyuki Ishidoya, Kazuhiro Tsuboi, Hiroaki Kondo, Kentaro Ishijima, Nobuyuki Aoki, Hidekazu Matsueda, and Kazuyuki Saito
Atmos. Chem. Phys., 24, 1059–1077, https://doi.org/10.5194/acp-24-1059-2024, https://doi.org/10.5194/acp-24-1059-2024, 2024
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A method evaluating techniques for carbon neutrality, such as carbon capture and storage (CCS), is important. This study presents a method to evaluate CO2 emissions from a cement plant based on atmospheric O2 and CO2 measurements. The method will also be useful for evaluating CO2 capture from flue gas at CCS plants, since the plants remove CO2 from the atmosphere without causing any O2 changes, just as cement plants do, differing only in the direction of CO2 exchange with the atmosphere.
Magdalena Pühl, Anke Roiger, Alina Fiehn, Alan M. Gorchov Negron, Eric A. Kort, Stefan Schwietzke, Ignacio Pisso, Amy Foulds, James Lee, James L. France, Anna E. Jones, Dave Lowry, Rebecca E. Fisher, Langwen Huang, Jacob Shaw, Prudence Bateson, Stephen Andrews, Stuart Young, Pamela Dominutti, Tom Lachlan-Cope, Alexandra Weiss, and Grant Allen
Atmos. Chem. Phys., 24, 1005–1024, https://doi.org/10.5194/acp-24-1005-2024, https://doi.org/10.5194/acp-24-1005-2024, 2024
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In April–May 2019 we carried out an airborne field campaign in the southern North Sea with the aim of studying methane emissions of offshore gas installations. We determined methane emissions from elevated methane measured downstream of the sampled installations. We compare our measured methane emissions with estimated methane emissions from national and global annual inventories. As a result, we find inconsistencies of inventories and large discrepancies between measurements and inventories.
Georgios I. Gkatzelis, Matthew M. Coggon, Chelsea E. Stockwell, Rebecca S. Hornbrook, Hannah Allen, Eric C. Apel, Megan M. Bela, Donald R. Blake, Ilann Bourgeois, Steven S. Brown, Pedro Campuzano-Jost, Jason M. St. Clair, James H. Crawford, John D. Crounse, Douglas A. Day, Joshua P. DiGangi, Glenn S. Diskin, Alan Fried, Jessica B. Gilman, Hongyu Guo, Johnathan W. Hair, Hannah S. Halliday, Thomas F. Hanisco, Reem Hannun, Alan Hills, L. Gregory Huey, Jose L. Jimenez, Joseph M. Katich, Aaron Lamplugh, Young Ro Lee, Jin Liao, Jakob Lindaas, Stuart A. McKeen, Tomas Mikoviny, Benjamin A. Nault, J. Andrew Neuman, John B. Nowak, Demetrios Pagonis, Jeff Peischl, Anne E. Perring, Felix Piel, Pamela S. Rickly, Michael A. Robinson, Andrew W. Rollins, Thomas B. Ryerson, Melinda K. Schueneman, Rebecca H. Schwantes, Joshua P. Schwarz, Kanako Sekimoto, Vanessa Selimovic, Taylor Shingler, David J. Tanner, Laura Tomsche, Krystal T. Vasquez, Patrick R. Veres, Rebecca Washenfelder, Petter Weibring, Paul O. Wennberg, Armin Wisthaler, Glenn M. Wolfe, Caroline C. Womack, Lu Xu, Katherine Ball, Robert J. Yokelson, and Carsten Warneke
Atmos. Chem. Phys., 24, 929–956, https://doi.org/10.5194/acp-24-929-2024, https://doi.org/10.5194/acp-24-929-2024, 2024
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This study reports emissions of gases and particles from wildfires. These emissions are related to chemical proxies that can be measured by satellite and incorporated into models to improve predictions of wildfire impacts on air quality and climate.
Jie Wang, Haichao Wang, Yee Jun Tham, Lili Ming, Zelong Zheng, Guizhen Fang, Cuizhi Sun, Zhenhao Ling, Jun Zhao, and Shaojia Fan
Atmos. Chem. Phys., 24, 977–992, https://doi.org/10.5194/acp-24-977-2024, https://doi.org/10.5194/acp-24-977-2024, 2024
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Many works report NO3 chemistry in inland regions while less target marine regions. We measured N2O5 and related species on a typical island and found intensive nighttime chemistry and rapid NO3 loss. NO contributed significantly to NO3 loss despite its sub-ppbv level, suggesting nocturnal NO3 reactions would be largely enhanced once free from NO emissions in the open ocean. This highlights the strong influences of urban outflow on downward marine areas in terms of nighttime chemistry.
Tanja J. Schuck, Johannes Degen, Eric Hintsa, Peter Hoor, Markus Jesswein, Timo Keber, Daniel Kunkel, Fred Moore, Florian Obersteiner, Matt Rigby, Thomas Wagenhäuser, Luke M. Western, Andreas Zahn, and Andreas Engel
Atmos. Chem. Phys., 24, 689–705, https://doi.org/10.5194/acp-24-689-2024, https://doi.org/10.5194/acp-24-689-2024, 2024
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We study the interhemispheric gradient of sulfur hexafluoride (SF6), a strong long-lived greenhouse gas. Its emissions are stronger in the Northern Hemisphere; therefore, mixing ratios in the Southern Hemisphere lag behind. Comparing the observations to a box model, the model predicts air in the Southern Hemisphere to be older. For a better agreement, the emissions used as model input need to be increased (and their spatial pattern changed), and we need to modify north–south transport.
Jérémy Gueffier, François Gheusi, Marie Lothon, Véronique Pont, Alban Philibert, Fabienne Lohou, Solène Derrien, Yannick Bezombes, Gilles Athier, Yves Meyerfeld, Antoine Vial, and Emmanuel Leclerc
Atmos. Chem. Phys., 24, 287–316, https://doi.org/10.5194/acp-24-287-2024, https://doi.org/10.5194/acp-24-287-2024, 2024
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This study investigates the link between weather regime and atmospheric composition at a Pyrenean observatory. Five years of meteorological data were synchronized on a daily basis and then, using a clustering method, separated into six groups of observation days, with most showing marked characteristics of different weather regimes (fair and disturbed weather, winter windstorms, foehn). Statistical differences in gas and particle concentrations appeared between the groups and are discussed.
Nathaniel Brockway, Peter K. Peterson, Katja Bigge, Kristian D. Hajny, Paul B. Shepson, Kerri A. Pratt, Jose D. Fuentes, Tim Starn, Robert Kaeser, Brian H. Stirm, and William R. Simpson
Atmos. Chem. Phys., 24, 23–40, https://doi.org/10.5194/acp-24-23-2024, https://doi.org/10.5194/acp-24-23-2024, 2024
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Bromine monoxide (BrO) strongly affects atmospheric chemistry in the springtime Arctic, yet there are still many uncertainties around its sources and recycling, particularly in the context of a rapidly changing Arctic. In this study, we observed BrO as a function of altitude above the Alaskan Arctic. We found that BrO was often most concentrated near the ground, confirming the ability of snow to produce and recycle reactive bromine, and identified four common vertical distributions of BrO.
Alina Fiehn, Maximilian Eckl, Julian Kostinek, Michał Gałkowski, Christoph Gerbig, Michael Rothe, Thomas Röckmann, Malika Menoud, Hossein Maazallahi, Martina Schmidt, Piotr Korbeń, Jarosław Neçki, Mila Stanisavljević, Justyna Swolkień, Andreas Fix, and Anke Roiger
Atmos. Chem. Phys., 23, 15749–15765, https://doi.org/10.5194/acp-23-15749-2023, https://doi.org/10.5194/acp-23-15749-2023, 2023
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During the CoMet mission in the Upper Silesian Coal Basin (USCB) ground-based and airborne air samples were taken and analyzed for the isotopic composition of CH4 to derive the mean signature of the USCB and source signatures of individual coal mines. Using δ2H signatures, the biogenic emissions from the USCB account for 15 %–50 % of total emissions, which is underestimated in common emission inventories. This demonstrates the importance of δ2H-CH4 observations for methane source apportionment.
Yifei Song, Chaoyang Xue, Yuanyuan Zhang, Pengfei Liu, Fengxia Bao, Xuran Li, and Yujing Mu
Atmos. Chem. Phys., 23, 15733–15747, https://doi.org/10.5194/acp-23-15733-2023, https://doi.org/10.5194/acp-23-15733-2023, 2023
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We present measurements of HONO flux and related parameters over an agricultural field during a whole growing season of summer maize. This dataset allows studies on the characteristics and influencing factors of soil HONO emissions, determination of HONO emission factors, estimation of total HONO emissions at a national scale, and the discussion on future environmental policies in terms of mitigating regional air pollution.
Can Ye, Keding Lu, Xuefei Ma, Wanyi Qiu, Shule Li, Xinping Yang, Chaoyang Xue, Tianyu Zhai, Yuhan Liu, Xuan Li, Yang Li, Haichao Wang, Zhaofeng Tan, Xiaorui Chen, Huabin Dong, Limin Zeng, Min Hu, and Yuanhang Zhang
Atmos. Chem. Phys., 23, 15455–15472, https://doi.org/10.5194/acp-23-15455-2023, https://doi.org/10.5194/acp-23-15455-2023, 2023
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In this study, combining comprehensive field measurements and a box model, we found NO2 conversion on the ground surface was the most important source for HONO production among the proposed heterogeneous and gas-phase HONO sources. In addition, HONO was found to evidently enhance O3 production and aggravate O3 pollution in summer in China. Our study improved our understanding of the relative importance of different HONO sources and the crucial role of HONO in O3 formation in polluted areas.
Yann Cohen, Didier Hauglustaine, Bastien Sauvage, Susanne Rohs, Patrick Konjari, Ulrich Bundke, Andreas Petzold, Valérie Thouret, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 23, 14973–15009, https://doi.org/10.5194/acp-23-14973-2023, https://doi.org/10.5194/acp-23-14973-2023, 2023
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The upper troposphere–lower stratosphere (UTLS) is a key region regarding the lower atmospheric composition. This study consists of a comprehensive evaluation of an up-to-date chemistry–climate model in this layer, using regular in situ measurements based on passenger aircraft. For this purpose, a specific software (Interpol-IAGOS) has been updated and made publicly available. The model reproduces the carbon monoxide peaks due to biomass burning over the continental tropics particularly well.
Yifan Jiang, Men Xia, Zhe Wang, Penggang Zheng, Yi Chen, and Tao Wang
Atmos. Chem. Phys., 23, 14813–14828, https://doi.org/10.5194/acp-23-14813-2023, https://doi.org/10.5194/acp-23-14813-2023, 2023
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This study provides the first estimate of high rates of formic acid (HCOOH) production from the photochemical aging of real ambient particles and demonstrates the potential importance of this pathway in the formation of HCOOH under ambient conditions. Incorporating this pathway significantly improved the performance of a widely used chemical model. Our solution irradiation experiments demonstrated the importance of nitrate photolysis in HCOOH production via the production of oxidants.
Xuelian Zhong, Hengqing Shen, Min Zhao, Ji Zhang, Yue Sun, Yuhong Liu, Yingnan Zhang, Ye Shan, Hongyong Li, Jiangshan Mu, Yu Yang, Yanqiu Nie, Jinghao Tang, Can Dong, Xinfeng Wang, Yujiao Zhu, Mingzhi Guo, Wenxing Wang, and Likun Xue
Atmos. Chem. Phys., 23, 14761–14778, https://doi.org/10.5194/acp-23-14761-2023, https://doi.org/10.5194/acp-23-14761-2023, 2023
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Nitrous acid (HONO) is vital for atmospheric oxidation. In research at Mount Lao, China, models revealed a significant unidentified marine HONO source. Overlooking this could skew our understanding of air quality and climate change. This finding emphasizes HONO’s importance in the coastal atmosphere, uncovering previously unnoticed interactions.
Steven Job Thomas, Toni Tykkä, Heidi Hellén, Federico Bianchi, and Arnaud P. Praplan
Atmos. Chem. Phys., 23, 14627–14642, https://doi.org/10.5194/acp-23-14627-2023, https://doi.org/10.5194/acp-23-14627-2023, 2023
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The study employed total ozone reactivity to demonstrate how emissions of Norway spruce readily react with ozone and could be a major ozone sink, particularly under stress. Additionally, this approach provided insight into the limitations of current analytical techniques that measure the compounds present or emitted into the atmosphere. The study shows how the technique used was not enough to measure all compounds emitted, and this could potentially underestimate various atmospheric processes.
Jinsol Kim, John B. Miller, Charles E. Miller, Scott J. Lehman, Sylvia E. Michel, Vineet Yadav, Nick E. Rollins, and William M. Berelson
Atmos. Chem. Phys., 23, 14425–14436, https://doi.org/10.5194/acp-23-14425-2023, https://doi.org/10.5194/acp-23-14425-2023, 2023
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In this study, we present the partitioning of CO2 signals from biogenic, petroleum and natural gas sources by combining CO, 13CO2 and 14CO2 measurements. Using measurements from flask air samples at three sites in the greater Los Angeles region, we find larger and positive contributions of biogenic signals in winter and smaller and negative contributions in summer. The largest contribution of natural gas combustion generally occurs in summer.
Robert Woodward-Massey, Roberto Sommariva, Lisa K. Whalley, Danny R. Cryer, Trevor Ingham, William J. Bloss, Stephen M. Ball, Sam Cox, James D. Lee, Chris P. Reed, Leigh R. Crilley, Louisa J. Kramer, Brian J. Bandy, Grant L. Forster, Claire E. Reeves, Paul S. Monks, and Dwayne E. Heard
Atmos. Chem. Phys., 23, 14393–14424, https://doi.org/10.5194/acp-23-14393-2023, https://doi.org/10.5194/acp-23-14393-2023, 2023
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Measurements of OH, HO2 and RO2 radicals and also OH reactivity were made at a UK coastal site and compared to calculations from a constrained box model utilising the Master Chemical Mechanism. The model agreement displayed a strong dependence on the NO concentration. An experimental budget analysis for OH, HO2, RO2 and total ROx demonstrated significant imbalances between HO2 and RO2 production rates. Ozone production rates were calculated from measured radicals and compared to modelled values.
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
Atmos. Chem. Phys., 23, 14349–14357, https://doi.org/10.5194/acp-23-14349-2023, https://doi.org/10.5194/acp-23-14349-2023, 2023
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This study provides ground-observational evidence that supports earlier suggestions that savanna fires are the main emitters and modulators of carbon monoxide gas in Africa. Using isotope-based techniques, the study has shown that about two-thirds of this gas is emitted from savanna fires, while for urban areas, in this case Nairobi, primary sources approach 100 %. The latter has implications for air quality policy, suggesting primary emissions such as traffic should be targeted.
Ziyan Guo, Keding Lu, Pengxiang Qiu, Mingyi Xu, and Zhaobing Guo
EGUsphere, https://doi.org/10.5194/egusphere-2023-2554, https://doi.org/10.5194/egusphere-2023-2554, 2023
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The formation of secondary sulfate in the atmosphere remains controversial, and it is urgent to seek for a new method to quantify different sulfate formation pathways. Due to their sensitivity for the reaction environment, Isotope fractionation has widely used in trace of atmospheric processes. In this work, the contributions of typical oxidation pathways of sulfate formation are calculated on the basis of laboratory simulation and field observation via sulfur and oxygen isotope fractionation.
Delaney B. Kilgour, Gordon A. Novak, Megan S. Claflin, Brian M. Lerner, and Timothy H. Bertram
EGUsphere, https://doi.org/10.5194/egusphere-2023-2210, https://doi.org/10.5194/egusphere-2023-2210, 2023
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Laboratory experiments with seawater mimics suggest ozone deposition to the surface ocean can be a source of reactive carbon to the marine atmosphere. We conduct both field and laboratory measurements to assess abiotic VOC composition and yields from ozonolysis of real surface seawater. We show that C5–C11 aldehydes contribute to the observed VOC emission flux. We estimate that VOC generated by the ozonolysis of surface seawater is competitive with biological VOC production and emission.
Clara M. Nussbaumer, Bryan K. Place, Qindan Zhu, Eva Y. Pfannerstill, Paul Wooldridge, Benjamin C. Schulze, Caleb Arata, Ryan Ward, Anthony Bucholtz, John H. Seinfeld, Allen H. Goldstein, and Ronald C. Cohen
Atmos. Chem. Phys., 23, 13015–13028, https://doi.org/10.5194/acp-23-13015-2023, https://doi.org/10.5194/acp-23-13015-2023, 2023
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NOx is a precursor to hazardous tropospheric ozone and can be emitted from various anthropogenic sources. It is important to quantify NOx emissions in urban environments to improve the local air quality, which still remains a challenge, as sources are heterogeneous in space and time. In this study, we calculate NOx emissions over Los Angeles, based on aircraft measurements in June 2021, and compare them to a local emission inventory, which we find mostly overpredicts the measured values.
Magdalena Okuljar, Olga Garmash, Miska Olin, Joni Kalliokoski, Hilkka Timonen, Jarkko V. Niemi, Pauli Paasonen, Jenni Kontkanen, Yanjun Zhang, Heidi Hellén, Heino Kuuluvainen, Minna Aurela, Hanna E. Manninen, Mikko Sipilä, Topi Rönkkö, Tuukka Petäjä, Markku Kulmala, Miikka Dal Maso, and Mikael Ehn
Atmos. Chem. Phys., 23, 12965–12983, https://doi.org/10.5194/acp-23-12965-2023, https://doi.org/10.5194/acp-23-12965-2023, 2023
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Highly oxygenated organic molecules (HOMs) form secondary organic aerosol that affects air quality and health. In this study, we demonstrate that in a moderately polluted city with abundant vegetation, the composition of HOMs is largely controlled by the effect of NOx on the biogenic volatile organic compound oxidation. Comparing the results from two nearby stations, we show that HOM composition and formation pathways can change considerably within small distances in urban environments.
Si-Wan Kim, Kyoung-Min Kim, Yujoo Jeong, Seunghwan Seo, Yeonsu Park, and Jeongyeon Kim
Atmos. Chem. Phys., 23, 12867–12886, https://doi.org/10.5194/acp-23-12867-2023, https://doi.org/10.5194/acp-23-12867-2023, 2023
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Surface ozone is a pollutant regulated for public health. This study derived surface ozone trends over South Korea from 2001 to 2021 and highlighted that South Korea has been a nonattainment area since 2010, based on the US EPA standard. However, the occurrences of high ozone condition decreased in spring during the COVID-19 pandemic, partly due to large reductions of ozone precursor concentrations in China and South Korea.
Zeyu Sun, Zheng Zong, Yang Tan, Chongguo Tian, Zeyu Liu, Fan Zhang, Rong Sun, Yingjun Chen, Jun Li, and Gan Zhang
Atmos. Chem. Phys., 23, 12851–12865, https://doi.org/10.5194/acp-23-12851-2023, https://doi.org/10.5194/acp-23-12851-2023, 2023
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This is the first report of ship-emitted nitrogen stable isotope composition (δ15N) of nitrogen oxides (NOx). The results showed that δ15N–NOx from ships was −18.5 ± 10.9 ‰ and increased monotonically with tightening emission regulations. The selective catalytic reduction system was the most vital factor. The temporal variation in δ15N–NOx was evaluated and can be used to select suitable δ15N–NOx for a more accurate assessment of the contribution of ship-emitted exhaust to atmospheric NOx.
Eva Y. Pfannerstill, Caleb Arata, Qindan Zhu, Benjamin C. Schulze, Roy Woods, John H. Seinfeld, Anthony Bucholtz, Ronald C. Cohen, and Allen H. Goldstein
Atmos. Chem. Phys., 23, 12753–12780, https://doi.org/10.5194/acp-23-12753-2023, https://doi.org/10.5194/acp-23-12753-2023, 2023
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The San Joaquin Valley is an agricultural area with poor air quality. Organic gases drive the formation of hazardous air pollutants. Agricultural emissions of these gases are not well understood and have rarely been quantified at landscape scale. By combining aircraft-based emission measurements with land cover information, we found mis- or unrepresented emission sources. Our results help in understanding of pollution sources and in improving predictions of air quality in agricultural regions.
Yao Yan Huang and D. James Donaldson
EGUsphere, https://doi.org/10.5194/egusphere-2023-1751, https://doi.org/10.5194/egusphere-2023-1751, 2023
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Ground-level ozone interacts at the lake-land boundary; this is important to our understanding and modelling of atmospheric chemistry and air pollution in the lower atmosphere. We show that a steep ozone gradient occurs year-round moving inland up to 1 km from the lake and that this gradient is influenced by seasonal factors on the local land environment, where more rural areas are greater affected seasonally.
Youwei Hong, Keran Zhang, Dan Liao, Gaojie Chen, Min Zhao, Yiling Lin, Xiaoting Ji, Ke Xu, Yu Wu, Ruilian Yu, Gongren Hu, Sung-Deuk Choi, Likun Xue, and Jinsheng Chen
Atmos. Chem. Phys., 23, 10795–10807, https://doi.org/10.5194/acp-23-10795-2023, https://doi.org/10.5194/acp-23-10795-2023, 2023
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Particle uptakes of HCHO and the impacts on PM2.5 and O3 production remain highly uncertain. Based on the investigation of co-occurring wintertime O3 and PM2.5 pollution in a coastal city of southeast China, we found enhanced heterogeneous formation of hydroxymethanesulfonate (HMS) and increased ROx concentrations and net O3 production rates. The findings of this study are helpful to better explore the mechanisms of key precursors for co-occurring PM2.5 and O3 pollution.
Foteini Stavropoulou, Katarina Vinković, Bert Kers, Marcel de Vries, Steven van Heuven, Piotr Korbeń, Martina Schmidt, Julia Wietzel, Pawel Jagoda, Jaroslav M. Necki, Jakub Bartyzel, Hossein Maazallahi, Malika Menoud, Carina van der Veen, Sylvia Walter, Béla Tuzson, Jonas Ravelid, Randulph Paulo Morales, Lukas Emmenegger, Dominik Brunner, Michael Steiner, Arjan Hensen, Ilona Velzeboer, Pim van den Bulk, Hugo Denier van der Gon, Antonio Delre, Maklawe Essonanawe Edjabou, Charlotte Scheutz, Marius Corbu, Sebastian Iancu, Denisa Moaca, Alin Scarlat, Alexandru Tudor, Ioana Vizireanu, Andreea Calcan, Magdalena Ardelean, Sorin Ghemulet, Alexandru Pana, Aurel Constantinescu, Lucian Cusa, Alexandru Nica, Calin Baciu, Cristian Pop, Andrei Radovici, Alexandru Mereuta, Horatiu Stefanie, Alexandru Dandocsi, Bas Hermans, Stefan Schwietzke, Daniel Zavala-Araiza, Huilin Chen, and Thomas Röckmann
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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In this study, we quantify CH4 emissions from onshore oil production sites in Romania at source and facility level using a combination of ground- and drone-based measurement techniques. We show that the total CH4 emissions in our studied areas are much higher than the emissions reported to UNFCCC, and up to three-quarters of the detected emissions are related to operational venting. Our results suggest that oil and gas production infrastructure in Romania holds a massive mitigation potential.
Chunxiang Ye, Shuzheng Guo, Weili Lin, Fangjie Tian, Jianshu Wang, Chong Zhang, Suzhen Chi, Yi Chen, Yingjie Zhang, Limin Zeng, Xin Li, Duo Bu, Jiacheng Zhou, and Weixiong Zhao
Atmos. Chem. Phys., 23, 10383–10397, https://doi.org/10.5194/acp-23-10383-2023, https://doi.org/10.5194/acp-23-10383-2023, 2023
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Online volatile organic compound (VOC) measurements by gas chromatography–mass spectrometry, with other O3 precursors, were used to identify key VOC and other key sources in Lhasa. Total VOCs (TVOCs), alkanes, and aromatics are half as abundant as in Beijing. Oxygenated VOCs (OVOCs) consist of 52 % of the TVOCs. Alkenes and OVOCs account for 80 % of the ozone formation potential. Aromatics dominate secondary organic aerosol potential. Positive matrix factorization decomposed residential sources.
Brandon Bottorff, Michelle M. Lew, Youngjun Woo, Pamela Rickly, Matthew D. Rollings, Benjamin Deming, Daniel C. Anderson, Ezra Wood, Hariprasad D. Alwe, Dylan B. Millet, Andrew Weinheimer, Geoff Tyndall, John Ortega, Sebastien Dusanter, Thierry Leonardis, James Flynn, Matt Erickson, Sergio Alvarez, Jean C. Rivera-Rios, Joshua D. Shutter, Frank Keutsch, Detlev Helmig, Wei Wang, Hannah M. Allen, Johnathan H. Slade, Paul B. Shepson, Steven Bertman, and Philip S. Stevens
Atmos. Chem. Phys., 23, 10287–10311, https://doi.org/10.5194/acp-23-10287-2023, https://doi.org/10.5194/acp-23-10287-2023, 2023
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The hydroxyl (OH), hydroperoxy (HO2), and organic peroxy (RO2) radicals play important roles in atmospheric chemistry and have significant air quality implications. Here, we compare measurements of OH, HO2, and total peroxy radicals (XO2) made in a remote forest in Michigan, USA, to predictions from a series of chemical models. Lower measured radical concentrations suggest that the models may be missing an important radical sink and overestimating the rate of ozone production in this forest.
Jenny Oh, Chubashini Shunthirasingham, Ying Duan Lei, Faqiang Zhan, Yuening Li, Abigaëlle Dalpé Castilloux, Amina Ben Chaaben, Zhe Lu, Kelsey Lee, Frank A. P. C. Gobas, Sabine Eckhardt, Nick Alexandrou, Hayley Hung, and Frank Wania
Atmos. Chem. Phys., 23, 10191–10205, https://doi.org/10.5194/acp-23-10191-2023, https://doi.org/10.5194/acp-23-10191-2023, 2023
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An emerging brominated flame retardant (BFR) called TBECH (1,2-dibromo-4-(1,2-dibromoethyl)cyclohexane) has never been produced or imported for use in Canada yet is found to be one of the most abundant gaseous BFRs in the Canadian atmosphere. The recorded spatial and temporal variability of TBECH suggest that the release from imported consumer products containing TBECH is the most likely explanation for its environmental occurrence in Canada.
Olivia E. Clifton, Donna Schwede, Christian Hogrefe, Jesse O. Bash, Sam Bland, Philip Cheung, Mhairi Coyle, Lisa Emberson, Johannes Flemming, Erick Fredj, Stefano Galmarini, Laurens Ganzeveld, Orestis Gazetas, Ignacio Goded, Christopher D. Holmes, László Horváth, Vincent Huijnen, Qian Li, Paul A. Makar, Ivan Mammarella, Giovanni Manca, J. William Munger, Juan L. Pérez-Camanyo, Jonathan Pleim, Limei Ran, Roberto San Jose, Sam J. Silva, Ralf Staebler, Shihan Sun, Amos P. K. Tai, Eran Tas, Timo Vesala, Tamás Weidinger, Zhiyong Wu, and Leiming Zhang
Atmos. Chem. Phys., 23, 9911–9961, https://doi.org/10.5194/acp-23-9911-2023, https://doi.org/10.5194/acp-23-9911-2023, 2023
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A primary sink of air pollutants is dry deposition. Dry deposition estimates differ across the models used to simulate atmospheric chemistry. Here, we introduce an effort to examine dry deposition schemes from atmospheric chemistry models. We provide our approach’s rationale, document the schemes, and describe datasets used to drive and evaluate the schemes. We also launch the analysis of results by evaluating against observations and identifying the processes leading to model–model differences.
Qindan Zhu, Bryan Place, Eva Y. Pfannerstill, Sha Tong, Huanxin Zhang, Jun Wang, Clara M. Nussbaumer, Paul Wooldridge, Benjamin C. Schulze, Caleb Arata, Anthony Bucholtz, John H. Seinfeld, Allen H. Goldstein, and Ronald C. Cohen
Atmos. Chem. Phys., 23, 9669–9683, https://doi.org/10.5194/acp-23-9669-2023, https://doi.org/10.5194/acp-23-9669-2023, 2023
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Nitrogen oxide (NOx) is a hazardous air pollutant, and it is the precursor of short-lived climate forcers like tropospheric ozone and aerosol particles. While NOx emissions from transportation has been strictly regulated, soil NOx emissions are overlooked. We use the airborne flux measurements to observe NOx emissions from highways and urban and cultivated soil land cover types. We show non-negligible soil NOx emissions, which are significantly underestimated in current model simulations.
Money Ossohou, Jonathan Edward Hickman, Lieven Clarisse, Pierre-François Coheur, Martin Van Damme, Marcellin Adon, Véronique Yoboué, Eric Gardrat, Maria Dias Alvès, and Corinne Galy-Lacaux
Atmos. Chem. Phys., 23, 9473–9494, https://doi.org/10.5194/acp-23-9473-2023, https://doi.org/10.5194/acp-23-9473-2023, 2023
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The updated analyses of ground-based concentrations and satellite total vertical columns of atmospheric ammonia help us to better understand 21st century ammonia dynamics in sub-Saharan Africa. We conclude that the drivers of trends are agriculture in the dry savanna of Katibougou, Mali; air temperature and agriculture in the wet savanna of Djougou, Benin, and Lamto, Côte d'Ivoire; and leaf area index, air temperature, residential, and agriculture in forests of Bomassa, Republic of Congo.
Hyeri Park, Jooil Kim, Haklim Choi, Sohyeon Geum, Yeaseul Kim, Rona L. Thompson, Jens Mühle, Peter K. Salameh, Christina M. Harth, Kieran M. Stanley, Simon O'Doherty, Paul J. Fraser, Peter G. Simmonds, Paul B. Krummel, Ray F. Weiss, Ronald G. Prinn, and Sunyoung Park
Atmos. Chem. Phys., 23, 9401–9411, https://doi.org/10.5194/acp-23-9401-2023, https://doi.org/10.5194/acp-23-9401-2023, 2023
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Based on atmospheric HFC-23 observations, the first estimate of post-CDM HFC-23 emissions in eastern Asia for 2008–2019 shows that these emissions contribute significantly to the global emissions rise. The observation-derived emissions were much larger than the bottom-up estimates expected to approach zero after 2015 due to national abatement activities. These discrepancies could be attributed to unsuccessful factory-level HFC-23 abatement and inaccurate quantification of emission reductions.
Philipp Eger, Theresa Mathes, Alex Zavarsky, and Lars Duester
Atmos. Chem. Phys., 23, 8769–8788, https://doi.org/10.5194/acp-23-8769-2023, https://doi.org/10.5194/acp-23-8769-2023, 2023
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We investigated the contribution of inland shipping to air pollution at the river Rhine in Germany. Land-based measurements of gaseous and particulate pollutants were carried out for more than 1 year to provide a realistic estimate for the exposure of people to air pollution close to the riverside. Emissions of nitrogen oxides and particulate matter relative to the amount of fuel used, as well as their dependence on ship size, engine type and operating conditions, were examined.
Imran A. Girach, Narendra Ojha, Prabha R. Nair, Kandula V. Subrahmanyam, Neelakantan Koushik, Mohammed M. Nazeer, Nadimpally Kiran Kumar, Surendran Nair Suresh Babu, Jos Lelieveld, and Andrea Pozzer
EGUsphere, https://doi.org/10.5194/egusphere-2023-1524, https://doi.org/10.5194/egusphere-2023-1524, 2023
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We investigated surface ozone variability at East Antarctica based on the measurements and EMAC global model simulations during austral summer. Nearly half of the surface ozone is found to be of stratospheric origin. The east coast of Antarctica acts as a stronger sink of ozone than surrounding regions. Photochemical loss of ozone is counterbalanced by downward transport of ozone. Study highlights intertwined role of chemistry and dynamics in governing the ozone variations over East Antarctica.
Hejun Hu, Haichao Wang, Keding Lu, Jie Wang, Zelong Zheng, Xuezhen Xu, Tianyu Zhai, Xiaorui Chen, Xiao Lu, Wenxing Fu, Xin Li, Limin Zeng, Min Hu, Yuanhang Zhang, and Shaojia Fan
Atmos. Chem. Phys., 23, 8211–8223, https://doi.org/10.5194/acp-23-8211-2023, https://doi.org/10.5194/acp-23-8211-2023, 2023
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Nitrate radical chemistry is critical to the degradation of volatile organic compounds (VOCs) and secondary organic aerosol formation. This work investigated the level, seasonal variation, and trend of nitrate radical reactivity towards volatile organic compounds (kNO3) in Beijing. We show the key role of isoprene and styrene in regulating seasonal variation in kNO3 and rebuild a long-term record of kNO3 based on the reported VOC measurements.
Eliane Gomes Alves, Raoni Aquino Santana, Cléo Quaresma Dias-Júnior, Santiago Botía, Tyeen Taylor, Ana Maria Yáñez-Serrano, Jürgen Kesselmeier, Efstratios Bourtsoukidis, Jonathan Williams, Pedro Ivo Lembo Silveira de Assis, Giordane Martins, Rodrigo de Souza, Sérgio Duvoisin Júnior, Alex Guenther, Dasa Gu, Anywhere Tsokankunku, Matthias Sörgel, Bruce Nelson, Davieliton Pinto, Shujiro Komiya, Diogo Martins Rosa, Bettina Weber, Cybelli Barbosa, Michelle Robin, Kenneth J. Feeley, Alvaro Duque, Viviana Londoño Lemos, Maria Paula Contreras, Alvaro Idarraga, Norberto López, Chad Husby, Brett Jestrow, and Iván Mauricio Cely Toro
Atmos. Chem. Phys., 23, 8149–8168, https://doi.org/10.5194/acp-23-8149-2023, https://doi.org/10.5194/acp-23-8149-2023, 2023
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Isoprene is emitted mainly by plants and can influence atmospheric chemistry and air quality. But, there are uncertainties in model emission estimates and follow-up atmospheric processes. In our study, with long-term observational datasets of isoprene and biological and environmental factors from central Amazonia, we show that isoprene emission estimates could be improved when biological processes were mechanistically incorporated into the model.
Thais Luarte, Victoria A. Gómez-Aburto, Ignacio Poblete-Castro, Eduardo Castro-Nallar, Nicolas Huneeus, Marco Molina-Montenegro, Claudia Egas, Germán Azcune, Andrés Pérez-Parada, Rainier Lohmann, Pernilla Bohlin-Nizzetto, Jordi Dachs, Susan Bengtson-Nash, Gustavo Chiang, Karla Pozo, and Cristóbal J. Galbán-Malagón
Atmos. Chem. Phys., 23, 8103–8118, https://doi.org/10.5194/acp-23-8103-2023, https://doi.org/10.5194/acp-23-8103-2023, 2023
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In the last 40 years, different research groups have reported on the atmospheric concentrations of persistent organic pollutants in Antarctica. In the present work, we make a compilation to understand the historical trends and estimate the atmospheric half-life of each compound. Of the compounds studied, HCB was the only one that showed no clear trend, while the rest of the studied compounds showed a significant decrease over time. This is consistent with results for polar and sub-polar zones.
Midhun George, Maria Dolores Andrés Hernández, Vladyslav Nenakhov, Yangzhuoran Liu, John Philip Burrows, Birger Bohn, Eric Förster, Florian Obersteiner, Andreas Zahn, Theresa Harlaß, Helmut Ziereis, Hans Schlager, Benjamin Schreiner, Flora Kluge, Katja Bigge, and Klaus Pfeilsticker
Atmos. Chem. Phys., 23, 7799–7822, https://doi.org/10.5194/acp-23-7799-2023, https://doi.org/10.5194/acp-23-7799-2023, 2023
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The applicability of photostationary steady-state (PSS) assumptions to estimate the amount of the sum of peroxy radicals (RO2*) during the EMeRGe airborne observations from the known radical chemistry and onboard measurements of RO2* precursors, photolysis frequencies, and other trace gases such as NOx and O3 was investigated. The comparison of the calculated RO2* with the actual measurements provides an insight into the main processes controlling their concentration in the air masses measured.
Ross Petersen, Thomas Holst, Meelis Mölder, Natascha Kljun, and Janne Rinne
Atmos. Chem. Phys., 23, 7839–7858, https://doi.org/10.5194/acp-23-7839-2023, https://doi.org/10.5194/acp-23-7839-2023, 2023
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We investigate variability in the vertical distribution of volatile organic compounds (VOCs) in boreal forest, determined through multiyear measurements at several heights in a boreal forest in Sweden. VOC source/sink seasonality in canopy was explored using these vertical profiles and with measurements from a collection of sonic anemometers on the station flux tower. Our results show seasonality in the source/sink distribution for several VOCs, such as monoterpenes and water-soluble compounds.
Wanyun Xu, Yuxuan Bian, Weili Lin, Yingjie Zhang, Yaru Wang, Zhiqiang Ma, Xiaoyi Zhang, Gen Zhang, Chunxiang Ye, and Xiaobin Xu
Atmos. Chem. Phys., 23, 7635–7652, https://doi.org/10.5194/acp-23-7635-2023, https://doi.org/10.5194/acp-23-7635-2023, 2023
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Tropospheric ozone (O3) and peroxyacetyl nitrate (PAN) are both photochemical pollutants harmful to the ecological environment and human health, especially in the Tibetan Plateau (TP). However, the factors determining their variations in the TP have not been comprehensively investigated. Results from field measurements and observation-based models revealed that day-to-day variations in O3 and PAN were in fact controlled by distinct physiochemical processes.
Megan E. McCabe, Ilana B. Pollack, Emily V. Fischer, Kathryn M. Steinmann, and Dana R. Caulton
Atmos. Chem. Phys., 23, 7479–7494, https://doi.org/10.5194/acp-23-7479-2023, https://doi.org/10.5194/acp-23-7479-2023, 2023
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Agriculture emissions, including those from beef and dairy cattle feeding operations, make up a large portion of the United States’ total greenhouse gas emissions, but many of these operations reside in areas where methane from oil and natural gas is prevalent, making it difficult to attribute methane in these areas. This work investigates two approaches to emission attribution for cattle feeding operations and provides guidance for emission attribution in other complicated regions.
Kai Qin, Wei Hu, Qin He, Fan Lu, and Jason Blake Cohen
EGUsphere, https://doi.org/10.5194/egusphere-2023-1210, https://doi.org/10.5194/egusphere-2023-1210, 2023
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Shanxi accounts for 10 % of the world’s coal production. This work computes CH4 emissions and uncertainty on a mine-by-mine basis, including underground, overground, and abandoned. This work uses a flux tower to observe and calculate emissions at one mine over 4 months. The half-hour variability and bias correction are propagated over the emissions dataset. Comparisons show the emissions are higher where mines are located, and regions with significant emissions but no mines are identified.
Haeyoung Lee, Wonick Seo, Shanlan Li, Soojeong Lee, Samuel Takele Kenea, and Sangwon Joo
Atmos. Chem. Phys., 23, 7141–7159, https://doi.org/10.5194/acp-23-7141-2023, https://doi.org/10.5194/acp-23-7141-2023, 2023
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We introduced three Korea Meteorological Administration (KMA) monitoring stations with monitoring systems and measurement uncertainty. We also analyzed the regional characteristics of CH4 at each KMA station. CH4 levels measured at KMA stations are compared to those measured at other Asian stations. From the long-term records of CH4 and δ13CH4 at AMY, we confirmed that the source of CH4xs changed from the past (2006 to 2010) to recent (2016 to 2020) years in East Asia.
Robert G. Ryan, Eloise A. Marais, Eleanor Gershenson-Smith, Robbie Ramsay, Jan-Peter Muller, Jan-Lukas Tirpitz, and Udo Frieß
Atmos. Chem. Phys., 23, 7121–7139, https://doi.org/10.5194/acp-23-7121-2023, https://doi.org/10.5194/acp-23-7121-2023, 2023
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We describe the first data retrieval from a newly installed instrument providing measurements of vertical profiles of air pollution over Central London during heatwaves in summer 2022. We use these observations with surface air quality network measurements to support interpretation that an exponential increase in biogenic emissions of isoprene during heatwaves provides the limiting ingredient for severe ozone pollution, leading to non-compliance with the national ozone air quality standard.
Zhouxing Zou, Qianjie Chen, Men Xia, Qi Yuan, Yi Chen, Yanan Wang, Enyu Xiong, Zhe Wang, and Tao Wang
Atmos. Chem. Phys., 23, 7057–7074, https://doi.org/10.5194/acp-23-7057-2023, https://doi.org/10.5194/acp-23-7057-2023, 2023
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We present OH observation and model simulation results at a coastal site in Hong Kong. The model predicted the OH concentration under high-NOx well but overpredicted it under low-NOx conditions. This implies an insufficient understanding of OH chemistry under low-NOx conditions. We show evidence of missing OH sinks as a possible cause of the overprediction.
Yaqin Gao, Hongli Wang, Lingling Yuan, Shengao Jing, Bin Yuan, Guofeng Shen, Liang Zhu, Abigail Koss, Yingjie Li, Qian Wang, Dan Dan Huang, Shuhui Zhu, Shikang Tao, Shengrong Lou, and Cheng Huang
Atmos. Chem. Phys., 23, 6633–6646, https://doi.org/10.5194/acp-23-6633-2023, https://doi.org/10.5194/acp-23-6633-2023, 2023
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A near-complete speciation of reactive organic gases from residential combustion was developed to get more insights into their atmospheric effects. Oxygenated species, higher hydrocarbons and nitrogen-containing species played larger roles in these emissions compared with common hydrocarbons. Based on the near-complete speciation, these emissions were largely underestimated, leading to more underestimation of their hydroxyl radical reactivity and secondary organic aerosol formation potential.
Guoxian Zhang, Renzhi Hu, Pinhua Xie, Changjin Hu, Xiaoyan Liu, Liujun Zhong, Haotian Cai, Bo Zhu, Shiyong Xia, Xiaofeng Huang, Xin Li, and Wenqing Liu
EGUsphere, https://doi.org/10.5194/egusphere-2023-550, https://doi.org/10.5194/egusphere-2023-550, 2023
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Comprehensive observations of HOx radicals were conducted at a coastal site in the Pearl River Delta. Radical chemistry was time-varyingly influenced by different air masses. Land mass (LAM) promotes a more active photochemical process, with daily averages of 7.1 × 106 cm−3 and 5.2 × 108 cm−3 for OH and HO2, respectively. The rapid oxidation process was accompanied by a higher diurnal HONO concentration, which influences the ozone-sensitive system and eventually magnifies the ozone background.
Katrin Müller, Jordis S. Tradowsky, Peter von der Gathen, Christoph Ritter, Sharon Patris, Justus Notholt, and Markus Rex
EGUsphere, https://doi.org/10.5194/egusphere-2023-1023, https://doi.org/10.5194/egusphere-2023-1023, 2023
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The Palau Atmospheric Observatory is introduced as an ideal site to detect changes in atmospheric composition and dynamics above the remote Tropical West Pacific. We focus on the ozone sounding program from 2016–2021, including El Nino 2016. The year-round high convective activity is reflected in dominant low tropospheric ozone and high relative humidity. The seasonal distribution of both constituents is unique compared to other tropical sites and modulated by the Intertropical Convergence Zone.
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Short summary
Predictions of global warming require predictions of how much CO2 will be taken up by the oceans, how much by land plants, and how much will stay in the atmosphere. Measurements of atmospheric oxygen (O2) help with these predictions if we also know the ratio of O2 release to CO2 uptake in land plants. We have measured this ratio in a midlatitude forest and find a lower value than the one in wide use. If truly applicable, our results call for a modest adjustment in the global carbon budget.
Predictions of global warming require predictions of how much CO2 will be taken up by the...
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