Articles | Volume 21, issue 23
https://doi.org/10.5194/acp-21-17907-2021
© Author(s) 2021. 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-21-17907-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Limitations of the radon tracer method (RTM) to estimate regional greenhouse gas (GHG) emissions – a case study for methane in Heidelberg
Ingeborg Levin
CORRESPONDING AUTHOR
Institut für Umweltphysik, Heidelberg University, INF 229, 69120
Heidelberg, Germany
Ute Karstens
ICOS ERIC Carbon Portal, Physical Geography and Ecosystem Science,
Lund University, Sölvegatan 12, 22362 Lund, Sweden
Samuel Hammer
Institut für Umweltphysik, Heidelberg University, INF 229, 69120
Heidelberg, Germany
ICOS Central Radiocarbon Laboratory, Heidelberg University, Berliner
Straße 53, 69120 Heidelberg, Germany
Julian DellaColetta
Institut für Umweltphysik, Heidelberg University, INF 229, 69120
Heidelberg, Germany
ICOS Central Radiocarbon Laboratory, Heidelberg University, Berliner
Straße 53, 69120 Heidelberg, Germany
Fabian Maier
Institut für Umweltphysik, Heidelberg University, INF 229, 69120
Heidelberg, Germany
ICOS Central Radiocarbon Laboratory, Heidelberg University, Berliner
Straße 53, 69120 Heidelberg, Germany
Maksym Gachkivskyi
Institut für Umweltphysik, Heidelberg University, INF 229, 69120
Heidelberg, Germany
ICOS Central Radiocarbon Laboratory, Heidelberg University, Berliner
Straße 53, 69120 Heidelberg, Germany
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We assess the uncertainty in continuous fossil fuel carbon dioxide (ffCO2) estimates derived from carbon monoxide (CO) observations and radiocarbon (14CO2) flask measurements from an urban and a rural site. This study provides the basis for using continuous CO-based ffCO2 observations in atmospheric transport inversion frameworks to derive ffCO2 emission estimates. We also compare the flask-based CO / ffCO2 ratios with modeled ratios to validate an emission inventory for central Europe.
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We investigate the usage of discrete radiocarbon (14C)-based fossil fuel carbon dioxide (ffCO2) concentration estimates vs. continuous carbon monoxide (CO)-based ffCO2 estimates to evaluate the seasonal cycle of ffCO2 emissions in an urban region with an inverse modeling framework. We find that the CO-based ffCO2 estimates allow us to reconstruct robust seasonal cycles, which show the distinct COVID-19 drawdown in 2020 and can be used to validate emission inventories.
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This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Fabian Maier, Eva Falge, Maksym Gachkivskyi, Stephan Henne, Ute Karstens, Dafina Kikaj, Ingeborg Levin, Alistair Manning, Christian Rödenbeck, and Christoph Gerbig
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The radioactive noble gas radon (222Rn) is a suitable natural tracer for atmospheric transport and mixing processes that can be used to validate and calibrate atmospheric transport models. However, this requires accurate estimates of the 222Rn flux from the soil into the atmosphere. In our study, we evaluate the reliability of process-based 222Rn flux maps for Europe using a 222Rn inversion. Our inversion results can give some indications on how to improve the process-based 222Rn flux maps.
Ann-Kristin Kunz, Lars Borchardt, Andreas Christen, Julian Della Coletta, Markus Eritt, Xochilt Gutiérrez, Josh Hashemi, Rainer Hilland, Armin Jordan, Richard Kneißl, Virgile Legendre, Ingeborg Levin, Susanne Preunkert, Pascal Rubli, Stavros Stagakis, and Samuel Hammer
EGUsphere, https://doi.org/10.5194/egusphere-2024-3175, https://doi.org/10.5194/egusphere-2024-3175, 2025
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We present, to our knowledge, the first relaxed eddy accumulation system explicitly tailored to a radiocarbon (14C)-based partitioning of fossil and non-fossil urban CO2 fluxes. Laboratory tests and in-depth quality and performance checks prove that the system meets the technical requirements. A pilot application on a tall-tower in the city of Zurich, Switzerland, demonstrates the ability to separate fossil and non-fossil CO2 fluxes within the typical precision of 14C measurements.
Carlos Gómez-Ortiz, Guillaume Monteil, Ute Karstens, and Marko Scholze
EGUsphere, https://doi.org/10.5194/egusphere-2024-3013, https://doi.org/10.5194/egusphere-2024-3013, 2025
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In 2024, an intensive sampling campaign is being conducted to improve fossil CO₂ emission estimates in Europe using 14C measurements. By testing different strategies for selecting air samples, this study shows that increasing sample frequency and carefully choosing samples based on their fossil fuel and nuclear content leads to more accurate results, reducing the uncertainty and bias of the estimates.
Camille Yver-Kwok, Michel Ramonet, Léonard Rivier, Jinghui Lian, Claudia Grossi, Roger Curcoll, Dafina Kikaj, Edward Chung, and Ute Karstens
EGUsphere, https://doi.org/10.5194/egusphere-2024-3107, https://doi.org/10.5194/egusphere-2024-3107, 2024
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Here, we use greenhouse gas and radon data from a tall tower in France to estimate their fluxes within the station footprint from January 2017 to December 2022 using the Radon Tracer Method. Using the latest radon exhalation maps and standardized radon measurements, we found the greenhouse gas fluxes to be in agreement with the literature. Compared to inventories, there is a general agreement except for carbon dioxide where we show that the biogenic fluxes are not well represented in the model.
Luiz A. T. Machado, Jürgen Kesselmeier, Santiago Botía, Hella van Asperen, Meinrat O. Andreae, Alessandro C. de Araújo, Paulo Artaxo, Achim Edtbauer, Rosaria R. Ferreira, Marco A. Franco, Hartwig Harder, Sam P. Jones, Cléo Q. Dias-Júnior, Guido G. Haytzmann, Carlos A. Quesada, Shujiro Komiya, Jost Lavric, Jos Lelieveld, Ingeborg Levin, Anke Nölscher, Eva Pfannerstill, Mira L. Pöhlker, Ulrich Pöschl, Akima Ringsdorf, Luciana Rizzo, Ana M. Yáñez-Serrano, Susan Trumbore, Wanda I. D. Valenti, Jordi Vila-Guerau de Arellano, David Walter, Jonathan Williams, Stefan Wolff, and Christopher Pöhlker
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Composite analysis of gas concentration before and after rainfall, during the day and night, gives insight into the complex relationship between trace gas variability and precipitation. The analysis helps us to understand the sources and sinks of trace gases within a forest ecosystem. It elucidates processes that are not discernible under undisturbed conditions and contributes to a deeper understanding of the trace gas life cycle and its intricate interactions with cloud dynamics in the Amazon.
Fabian Maier, Ingeborg Levin, Sébastien Conil, Maksym Gachkivskyi, Hugo Denier van der Gon, and Samuel Hammer
Atmos. Chem. Phys., 24, 8205–8223, https://doi.org/10.5194/acp-24-8205-2024, https://doi.org/10.5194/acp-24-8205-2024, 2024
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We assess the uncertainty in continuous fossil fuel carbon dioxide (ffCO2) estimates derived from carbon monoxide (CO) observations and radiocarbon (14CO2) flask measurements from an urban and a rural site. This study provides the basis for using continuous CO-based ffCO2 observations in atmospheric transport inversion frameworks to derive ffCO2 emission estimates. We also compare the flask-based CO / ffCO2 ratios with modeled ratios to validate an emission inventory for central Europe.
Fabian Maier, Christian Rödenbeck, Ingeborg Levin, Christoph Gerbig, Maksym Gachkivskyi, and Samuel Hammer
Atmos. Chem. Phys., 24, 8183–8203, https://doi.org/10.5194/acp-24-8183-2024, https://doi.org/10.5194/acp-24-8183-2024, 2024
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We investigate the usage of discrete radiocarbon (14C)-based fossil fuel carbon dioxide (ffCO2) concentration estimates vs. continuous carbon monoxide (CO)-based ffCO2 estimates to evaluate the seasonal cycle of ffCO2 emissions in an urban region with an inverse modeling framework. We find that the CO-based ffCO2 estimates allow us to reconstruct robust seasonal cycles, which show the distinct COVID-19 drawdown in 2020 and can be used to validate emission inventories.
Michael Steiner, Wouter Peters, Ingrid Luijkx, Stephan Henne, Huilin Chen, Samuel Hammer, and Dominik Brunner
Atmos. Chem. Phys., 24, 2759–2782, https://doi.org/10.5194/acp-24-2759-2024, https://doi.org/10.5194/acp-24-2759-2024, 2024
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The Paris Agreement increased interest in estimating greenhouse gas (GHG) emissions of individual countries, but top-down emission estimation is not yet considered policy-relevant. It is therefore paramount to reduce large errors and to build systems that are based on the newest atmospheric transport models. In this study, we present the first application of ICON-ART in the inverse modeling of GHG fluxes with an ensemble Kalman filter and present our results for European CH4 emissions.
Zhendong Wu, Alex Vermeulen, Yousuke Sawa, Ute Karstens, Wouter Peters, Remco de Kok, Xin Lan, Yasuyuki Nagai, Akinori Ogi, and Oksana Tarasova
Atmos. Chem. Phys., 24, 1249–1264, https://doi.org/10.5194/acp-24-1249-2024, https://doi.org/10.5194/acp-24-1249-2024, 2024
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This study focuses on exploring the differences in calculating global surface CO2 and its growth rate, considering the impact of analysis methodologies and site selection. Our study reveals that the current global CO2 network has a good capacity to represent global surface CO2 and its growth rate, as well as trends in atmospheric CO2 mass changes. However, small differences exist in different analyses due to the impact of methodology and site selection.
Christian Rödenbeck, Karina E. Adcock, Markus Eritt, Maksym Gachkivskyi, Christoph Gerbig, Samuel Hammer, Armin Jordan, Ralph F. Keeling, Ingeborg Levin, Fabian Maier, Andrew C. Manning, Heiko Moossen, Saqr Munassar, Penelope A. Pickers, Michael Rothe, Yasunori Tohjima, and Sönke Zaehle
Atmos. Chem. Phys., 23, 15767–15782, https://doi.org/10.5194/acp-23-15767-2023, https://doi.org/10.5194/acp-23-15767-2023, 2023
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The carbon dioxide content of the Earth atmosphere is increasing due to human emissions from burning of fossil fuels, causing global climate change. The strength of the fossil-fuel emissions is estimated by inventories based on energy data, but independent validation of these inventories has been recommended by the Intergovernmental Panel on Climate Change. Here we investigate the potential to validate inventories based on measurements of small changes in the atmospheric oxygen content.
Douglas E. J. Worthy, Michele K. Rauh, Lin Huang, Felix R. Vogel, Alina Chivulescu, Kenneth A. Masarie, Ray L. Langenfelds, Paul B. Krummel, Colin E. Allison, Andrew M. Crotwell, Monica Madronich, Gabrielle Pétron, Ingeborg Levin, Samuel Hammer, Sylvia Michel, Michel Ramonet, Martina Schmidt, Armin Jordan, Heiko Moossen, Michael Rothe, Ralph Keeling, and Eric J. Morgan
Atmos. Meas. Tech., 16, 5909–5935, https://doi.org/10.5194/amt-16-5909-2023, https://doi.org/10.5194/amt-16-5909-2023, 2023
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Network compatibility is important for inferring greenhouse gas fluxes at global or regional scales. This study is the first assessment of the measurement agreement among seven individual programs within the World Meteorological Organization community. It compares co-located flask air measurements at the Alert Observatory in Canada over a 17-year period. The results provide stronger confidence in the uncertainty estimation while using those datasets in various data interpretation applications.
Alessandro Zanchetta, Linda M. J. Kooijmans, Steven van Heuven, Andrea Scifo, Hubertus A. Scheeren, Ivan Mammarella, Ute Karstens, Jin Ma, Maarten Krol, and Huilin Chen
Biogeosciences, 20, 3539–3553, https://doi.org/10.5194/bg-20-3539-2023, https://doi.org/10.5194/bg-20-3539-2023, 2023
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Carbonyl sulfide (COS) has been suggested as a tool to estimate carbon dioxide (CO2) uptake by plants during photosynthesis. However, understanding its sources and sinks is critical to preventing biases in this estimate. Combining observations and models, this study proves that regional sources occasionally influence the measurements at the 60 m tall Lutjewad tower (1 m a.s.l.; 53°24′ N, 6°21′ E) in the Netherlands. Moreover, it estimates nighttime COS fluxes to be −3.0 ± 2.6 pmol m−2 s−1.
Ida Storm, Ute Karstens, Claudio D'Onofrio, Alex Vermeulen, and Wouter Peters
Atmos. Chem. Phys., 23, 4993–5008, https://doi.org/10.5194/acp-23-4993-2023, https://doi.org/10.5194/acp-23-4993-2023, 2023
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In this study, we evaluate what is in the influence regions of the ICOS atmospheric measurement stations to gain insight into what land cover types and land-cover-associated fluxes the network represents. Subsequently, insights about strengths, weaknesses, and potential gaps can assist in future network expansion decisions. The network is concentrated in central Europe, which leads to a general overrepresentation of coniferous forest and cropland and underrepresentation of grass and shrubland.
Saqr Munassar, Guillaume Monteil, Marko Scholze, Ute Karstens, Christian Rödenbeck, Frank-Thomas Koch, Kai U. Totsche, and Christoph Gerbig
Atmos. Chem. Phys., 23, 2813–2828, https://doi.org/10.5194/acp-23-2813-2023, https://doi.org/10.5194/acp-23-2813-2023, 2023
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Using different transport models results in large errors in optimized fluxes in the atmospheric inversions. Boundary conditions and inversion system configurations lead to a smaller but non-negligible impact. The findings highlight the importance to validate transport models for further developments but also to properly account for such errors in inverse modelling. This will help narrow the convergence of gas estimates reported in the scientific literature from different inversion frameworks.
Auke M. van der Woude, Remco de Kok, Naomi Smith, Ingrid T. Luijkx, Santiago Botía, Ute Karstens, Linda M. J. Kooijmans, Gerbrand Koren, Harro A. J. Meijer, Gert-Jan Steeneveld, Ida Storm, Ingrid Super, Hubertus A. Scheeren, Alex Vermeulen, and Wouter Peters
Earth Syst. Sci. Data, 15, 579–605, https://doi.org/10.5194/essd-15-579-2023, https://doi.org/10.5194/essd-15-579-2023, 2023
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To monitor the progress towards the CO2 emission goals set out in the Paris Agreement, the European Union requires an independent validation of emitted CO2. For this validation, atmospheric measurements of CO2 can be used, together with first-guess estimates of CO2 emissions and uptake. To quickly inform end users, it is imperative that this happens in near real-time. To aid these efforts, we create estimates of European CO2 exchange at high resolution in near real time.
Simone M. Pieber, Béla Tuzson, Stephan Henne, Ute Karstens, Christoph Gerbig, Frank-Thomas Koch, Dominik Brunner, Martin Steinbacher, and Lukas Emmenegger
Atmos. Chem. Phys., 22, 10721–10749, https://doi.org/10.5194/acp-22-10721-2022, https://doi.org/10.5194/acp-22-10721-2022, 2022
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Understanding regional greenhouse gas emissions into the atmosphere is a prerequisite to mitigate climate change. In this study, we investigated the regional contributions of carbon dioxide (CO2) at the location of the high Alpine observatory Jungfraujoch (JFJ, Switzerland, 3580 m a.s.l.). To this purpose, we combined receptor-oriented atmospheric transport simulations for CO2 concentration in the period 2009–2017 with stable carbon isotope (δ13C–CO2) information.
Fabian Maier, Christoph Gerbig, Ingeborg Levin, Ingrid Super, Julia Marshall, and Samuel Hammer
Geosci. Model Dev., 15, 5391–5406, https://doi.org/10.5194/gmd-15-5391-2022, https://doi.org/10.5194/gmd-15-5391-2022, 2022
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We show that the default representation of point source emissions in WRF–STILT leads to large overestimations when modelling fossil fuel CO2 concentrations for a 30 m high observation site during stable atmospheric conditions. We therefore introduce a novel point source modelling approach in WRF-STILT that takes into account their effective emission heights and results in a much better agreement with observations.
Stefan Röttger, Annette Röttger, Claudia Grossi, Arturo Vargas, Ute Karstens, Giorgia Cinelli, Edward Chung, Dafina Kikaj, Chris Rennick, Florian Mertes, and Ileana Radulescu
Adv. Geosci., 57, 37–47, https://doi.org/10.5194/adgeo-57-37-2022, https://doi.org/10.5194/adgeo-57-37-2022, 2022
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Radon gas is the largest source of public exposure to naturally occurring radioactivity. Radon can also be used, as a tracer to improve indirectly the estimates of greenhouse gases important for supporting successful GHG mitigation strategies.
Both climate and radiation protection research communities need improved traceable low-level atmospheric radon measurements. The EMPIR project 19ENV01 traceRadon started to provide the necessary measurement infrastructure and transfer standards.
Antoine Berchet, Espen Sollum, Rona L. Thompson, Isabelle Pison, Joël Thanwerdas, Grégoire Broquet, Frédéric Chevallier, Tuula Aalto, Adrien Berchet, Peter Bergamaschi, Dominik Brunner, Richard Engelen, Audrey Fortems-Cheiney, Christoph Gerbig, Christine D. Groot Zwaaftink, Jean-Matthieu Haussaire, Stephan Henne, Sander Houweling, Ute Karstens, Werner L. Kutsch, Ingrid T. Luijkx, Guillaume Monteil, Paul I. Palmer, Jacob C. A. van Peet, Wouter Peters, Philippe Peylin, Elise Potier, Christian Rödenbeck, Marielle Saunois, Marko Scholze, Aki Tsuruta, and Yuanhong Zhao
Geosci. Model Dev., 14, 5331–5354, https://doi.org/10.5194/gmd-14-5331-2021, https://doi.org/10.5194/gmd-14-5331-2021, 2021
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We present here the Community Inversion Framework (CIF) to help rationalize development efforts and leverage the strengths of individual inversion systems into a comprehensive framework. The CIF is a programming protocol to allow various inversion bricks to be exchanged among researchers.
The ensemble of bricks makes a flexible, transparent and open-source Python-based tool. We describe the main structure and functionalities and demonstrate it in a simple academic case.
Ana Maria Roxana Petrescu, Matthew J. McGrath, Robbie M. Andrew, Philippe Peylin, Glen P. Peters, Philippe Ciais, Gregoire Broquet, Francesco N. Tubiello, Christoph Gerbig, Julia Pongratz, Greet Janssens-Maenhout, Giacomo Grassi, Gert-Jan Nabuurs, Pierre Regnier, Ronny Lauerwald, Matthias Kuhnert, Juraj Balkovič, Mart-Jan Schelhaas, Hugo A. C. Denier van der
Gon, Efisio Solazzo, Chunjing Qiu, Roberto Pilli, Igor B. Konovalov, Richard A. Houghton, Dirk Günther, Lucia Perugini, Monica Crippa, Raphael Ganzenmüller, Ingrid T. Luijkx, Pete Smith, Saqr Munassar, Rona L. Thompson, Giulia Conchedda, Guillaume Monteil, Marko Scholze, Ute Karstens, Patrick Brockmann, and Albertus Johannes Dolman
Earth Syst. Sci. Data, 13, 2363–2406, https://doi.org/10.5194/essd-13-2363-2021, https://doi.org/10.5194/essd-13-2363-2021, 2021
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This study is topical and provides a state-of-the-art scientific overview of data availability from bottom-up and top-down CO2 fossil emissions and CO2 land fluxes in the EU27+UK. The data integrate recent emission inventories with ecosystem data, land carbon models and regional/global inversions for the European domain, aiming at reconciling CO2 estimates with official country-level UNFCCC national GHG inventories in support to policy and facilitating real-time verification procedures.
Guillaume Monteil, Grégoire Broquet, Marko Scholze, Matthew Lang, Ute Karstens, Christoph Gerbig, Frank-Thomas Koch, Naomi E. Smith, Rona L. Thompson, Ingrid T. Luijkx, Emily White, Antoon Meesters, Philippe Ciais, Anita L. Ganesan, Alistair Manning, Michael Mischurow, Wouter Peters, Philippe Peylin, Jerôme Tarniewicz, Matt Rigby, Christian Rödenbeck, Alex Vermeulen, and Evie M. Walton
Atmos. Chem. Phys., 20, 12063–12091, https://doi.org/10.5194/acp-20-12063-2020, https://doi.org/10.5194/acp-20-12063-2020, 2020
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The paper presents the first results from the EUROCOM project, a regional atmospheric inversion intercomparison exercise involving six European research groups. It aims to produce an estimate of the net carbon flux between the European terrestrial ecosystems and the atmosphere for the period 2006–2015, based on constraints provided by observed CO2 concentrations and using inverse modelling techniques. The use of six different models enables us to investigate the robustness of the results.
Ingeborg Levin, Ute Karstens, Markus Eritt, Fabian Maier, Sabrina Arnold, Daniel Rzesanke, Samuel Hammer, Michel Ramonet, Gabriela Vítková, Sebastien Conil, Michal Heliasz, Dagmar Kubistin, and Matthias Lindauer
Atmos. Chem. Phys., 20, 11161–11180, https://doi.org/10.5194/acp-20-11161-2020, https://doi.org/10.5194/acp-20-11161-2020, 2020
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Based on observations and Stochastic Time-Inverted Lagrangian Transport (STILT) footprint modelling, a sampling strategy has been developed for tall tower stations of the Integrated Carbon Observation System (ICOS) research infrastructure atmospheric station network. This strategy allows independent quality control of in situ measurements, provides representative coverage of the influence area of the sites, and is capable of automated targeted sampling of fossil fuel CO2 emission hotspots.
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Short summary
The radon tracer method is applied to atmospheric methane and radon observations from the upper Rhine valley to independently estimate methane emissions from the region. Comparison of our top-down results with bottom-up inventory data requires high-resolution footprint modelling and representative radon flux data. In agreement with inventories, observed emissions decreased, but only until 2005. A limitation of this method is that point-source emissions are not captured or not fully captured.
The radon tracer method is applied to atmospheric methane and radon observations from the upper...
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