Articles | Volume 17, issue 9
https://doi.org/10.5194/amt-17-2687-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/amt-17-2687-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
07 May 2024
Research article |
| 07 May 2024
| 07 May 2024
Extraction, purification, and clumped isotope analysis of methane (Δ13CDH3 and Δ12CD2H2) from sources and the atmosphere
Malavika Sivan
CORRESPONDING AUTHOR
Institute for Marine and Atmospheric research Utrecht (IMAU), Utrecht University, Utrecht, the Netherlands
Thomas Röckmann
Institute for Marine and Atmospheric research Utrecht (IMAU), Utrecht University, Utrecht, the Netherlands
Carina van der Veen
Institute for Marine and Atmospheric research Utrecht (IMAU), Utrecht University, Utrecht, the Netherlands
Maria Elena Popa
Institute for Marine and Atmospheric research Utrecht (IMAU), Utrecht University, Utrecht, the Netherlands
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Judith Tettenborn, Daniel Zavala-Araiza, Daan Stroeken, Hossein Maazallahi, Carina van der Veen, Arjan Hensen, Ilona Velzeboer, Pim van den Bulk, Felix Vogel, Lawson Gillespie, Sebastien Ars, James France, David Lowry, Rebecca Fisher, and Thomas Röckmann
Atmos. Meas. Tech., 18, 3569–3584, https://doi.org/10.5194/amt-18-3569-2025, https://doi.org/10.5194/amt-18-3569-2025, 2025
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Measurements of methane with vehicle-based sensors are an effective method to identify and quantify leaks from urban gas distribution systems. We deliberately released methane in different environments and calibrated the response of different methane analysers when they transected the plumes in a vehicle. We derived an improved statistical function for consistent emission estimations using different instruments. Repeated transects reduce the uncertainty in emission rate estimates.
Paul Waldmann, Max Eckl, Leon Knez, Klaus-Dirk Gottschaldt, Alina Fiehn, Christian Mallaun, Michal Galkowski, Christoph Kiemle, Ronald Hutjes, Thomas Röckmann, Huilin Chen, and Anke Roiger
EGUsphere, https://doi.org/10.5194/egusphere-2025-3297, https://doi.org/10.5194/egusphere-2025-3297, 2025
This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
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Nitrous oxide and methane emissions from agriculture need to be reduced, therefore emissions must be understood to effectively mitigate them. This is the first approach to measure those emissions aircraft-based, to assess their magnitude and drivers. We identified emission hotspots and temporal changes in agricultural emissions in the Netherlands. Our approach is applicable to further greenhouse gas emitters, therefore it builds a step towards more comprehensive emission quantification.
Lison Soussaintjean, Jochen Schmitt, Joël Savarino, J. Andy Menking, Edward J. Brook, Barbara Seth, Vladimir Lipenkov, Thomas Röckmann, and Hubertus Fischer
EGUsphere, https://doi.org/10.5194/egusphere-2025-3108, https://doi.org/10.5194/egusphere-2025-3108, 2025
This preprint is open for discussion and under review for Biogeosciences (BG).
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Nitrous oxide (N2O) produced in dust-rich Antarctic ice complicates the reconstruction of past atmospheric levels from ice core records. Using isotope analysis, we show that N2O forms from two nitrogen precursors, one being nitrate. For the first time, we demonstrate that the site preference (SP) of N2O reflects the isotopic difference between these precursors, not the production pathway, which challenges the common interpretation of SP.
Getachew Agmuas Adnew, Gerbrand Koren, Neha Mehendale, Sergey Gromov, Maarten Krol, and Thomas Röckmann
Atmos. Meas. Tech., 18, 2701–2719, https://doi.org/10.5194/amt-18-2701-2025, https://doi.org/10.5194/amt-18-2701-2025, 2025
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This study presents high-precision measurements of ∆′17O(CO2). Key findings include the extension of the N2O–∆′17O correlation to the upper troposphere and the identification of significant differences in the N2O–∆′17O slope in StratoClim samples. Additionally, the ∆′17O measurements are used to estimate global stratospheric production and surface removal of ∆′17O, providing an independent estimate of global vegetation CO2 exchange.
Sara M. Defratyka, Julianne M. Fernandez, Getachew A. Adnew, Guannan Dong, Peter M. J. Douglas, Daniel L. Eldridge, Giuseppe Etiope, Thomas Giunta, Mojhgan A. Haghnegahdar, Alexander N. Hristov, Nicole Hultquist, Iñaki Vadillo, Josue Jautzy, Ji-Hyun Kim, Jabrane Labidi, Ellen Lalk, Wil Leavitt, Jiawen Li, Li-Hung Lin, Jiarui Liu, Lucia Ojeda, Shuhei Ono, Jeemin Rhim, Thomas Röckmann, Barbara Sherwood Lollar, Malavika Sivan, Jiayang Sun, Gregory T. Ventura, David T. Wang, Edward D. Young, Naizhong Zhang, and Tim Arnold
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2025-41, https://doi.org/10.5194/essd-2025-41, 2025
Preprint under review for ESSD
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Measurement of methane’s doubly substituted isotopologues at natural abundances holds promise for better constraining the Earth’s atmospheric CH4 budget. We compiled 1475 measurements from field samples and laboratory experiments, conducted since 2014, to facilitate the differentiation of CH4 formation pathways and processes, to identify existing gaps limiting application of Δ13CH3D and Δ12CH2D2, and to develop isotope ratio source signature inputs for global CH4 flux modelling.
Bibhasvata Dasgupta, Malika Menoud, Carina van der Veen, Ingeborg Levin, Cora Veidt, Heiko Moossen, Sylvia Englund Michel, Peter Sperlich, Shinji Morimoto, Ryo Fujita, Taku Umezawa, Stephen Matthew Platt, Christine Groot Zwaaftink, Cathrine Lund Myhre, Rebecca Fisher, David Lowry, Euan Nisbet, James France, Ceres Woolley Maisch, Gordon Brailsford, Rowena Moss, Daisuke Goto, Sudhanshu Pandey, Sander Houweling, Nicola Warwick, and Thomas Röckmann
EGUsphere, https://doi.org/10.5194/egusphere-2025-2439, https://doi.org/10.5194/egusphere-2025-2439, 2025
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We combined long-term methane mole fraction and isotope measurements from eight laboratories that sample high-latitude stations to compare, offset correct and harmonise the datasets into a hemisphere merged timeseries. Because each laboratory uses slightly different methods, we adjusted the data to make it directly comparable. This allowed us to create a consistent record of atmospheric methane concentration and its isotopes from 1988 to 2023.
Gerrit Kuhlmann, Foteini Stavropoulou, Stefan Schwietzke, Daniel Zavala-Araiza, Andrew Thorpe, Andreas Hueni, Lukas Emmenegger, Andreea Calcan, Thomas Röckmann, and Dominik Brunner
Atmos. Chem. Phys., 25, 5371–5385, https://doi.org/10.5194/acp-25-5371-2025, https://doi.org/10.5194/acp-25-5371-2025, 2025
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A measurement campaign in 2019 found that methane emissions from oil and gas in Romania were significantly higher than reported. In 2021, our follow-up campaign using airborne remote sensing showed a marked decreases in emissions by 20 %–60 % due to improved infrastructure. The study highlights the importance of measurement-based emission monitoring and illustrates the value of a multi-scale assessment integrating ground-based observations with large-scale airborne remote sensing campaigns.
Tanja J. Schuck, Johannes Degen, Timo Keber, Katharina Meixner, Thomas Wagenhäuser, Mélanie Ghysels, Georges Durry, Nadir Amarouche, Alessandro Zanchetta, Steven van Heuven, Huilin Chen, Johannes C. Laube, Sophie L. Baartman, Carina van der Veen, Maria Elena Popa, and Andreas Engel
Atmos. Chem. Phys., 25, 4333–4348, https://doi.org/10.5194/acp-25-4333-2025, https://doi.org/10.5194/acp-25-4333-2025, 2025
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A balloon was launched in 2021 in the Arctic to carry instruments for trace gas measurements up to 32 km. One purpose was to compare measurement techniques. We focus on the major greenhouse gases. To measure these, air was sampled with the AirCore technique and with flask sampling, and samples were analysed after the flight. In flight, observations were done with an optical method. In a companion paper, we report on observations of chlorine and bromine containing trace gases.
Robbert Petrus Johannes Moonen, Getachew Agmuas Adnew, Jordi Vilà-Guerau de Arellano, Oscar Karel Hartogensis, David Joan Bonell Fontas, Shujiro Komiya, Sam P. Jones, and Thomas Röckmann
EGUsphere, https://doi.org/10.5194/egusphere-2025-452, https://doi.org/10.5194/egusphere-2025-452, 2025
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Understory ejections are distinct turbulent features emerging in prime tall forest ecosystems. We share a method to isolate understory ejections based on H2O-CO2 anomalie quadrants. From these, we calculate the flux contributions of understory ejections and all flux quadrants. In addition we show that a distinctly depleted isotopic composition can be found in the ejected water vapour. Finally, we explored the role of clouds as a potential trigger for understory ejections.
Hossein Maazallahi, Foteini Stavropoulou, Samuel Jonson Sutanto, Michael Steiner, Dominik Brunner, Mariano Mertens, Patrick Jöckel, Antoon Visschedijk, Hugo Denier van der Gon, Stijn Dellaert, Nataly Velandia Salinas, Stefan Schwietzke, Daniel Zavala-Araiza, Sorin Ghemulet, Alexandru Pana, Magdalena Ardelean, Marius Corbu, Andreea Calcan, Stephen A. Conley, Mackenzie L. Smith, and Thomas Röckmann
Atmos. Chem. Phys., 25, 1497–1511, https://doi.org/10.5194/acp-25-1497-2025, https://doi.org/10.5194/acp-25-1497-2025, 2025
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This article presents insights from airborne in situ measurements collected during the ROmanian Methane Emissions from Oil and gas (ROMEO) campaign supported by two models. Results reveal Romania's oil and gas methane emissions were significantly under-reported to the United Nations Framework Convention on Climate Change (UNFCCC) in 2019. A large underestimation was also found in the Emissions Database for Global Atmospheric Research (EDGAR) v7.0 for the study domain in the same year.
Sophie L. Baartman, Steven M. Driever, Maarten Wassenaar, Linda M. J. Kooijmans, Nerea Ubierna Lopez, Leon Mossink, Maria E. Popa, Ara Cho, Lisa Wingate, Thomas Röckmann, Steven M. A. C. van Heuven, and Maarten C. Krol
EGUsphere, https://doi.org/10.5194/egusphere-2025-215, https://doi.org/10.5194/egusphere-2025-215, 2025
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Carbonyl sulfide (COS) and carbon dioxide (CO2) uptake fluxes and isotope discrimination was measured in sunflower and papyrus plants, using a plant chamber approach and varying light availability. COS and CO2 isotope discrimination in plants have never been jointly measured before. COS isotope discrimination did not differ between the species, nor with changing light. CO2 fluxes and isotope values provided additional useful information for data interpretation.
Johannes C. Laube, Tanja J. Schuck, Huilin Chen, Markus Geldenhuys, Steven van Heuven, Timo Keber, Maria Elena Popa, Elinor Tuffnell, Bärbel Vogel, Thomas Wagenhäuser, Alessandro Zanchetta, and Andreas Engel
EGUsphere, https://doi.org/10.5194/egusphere-2024-4034, https://doi.org/10.5194/egusphere-2024-4034, 2025
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A large balloon was launched in summer 2021 in the Arctic to carry instruments for trace gas measurements up to 32 km, above the reach of aircraft. The main aims were to evaluate different techniques and atmospheric processes. We focus on halogenated greenhouse gases and ozone-depleting substances. For this, air was collected with the AirCore technique and a cryogenic air sampler and measured after the flight. A companion paper reports observations of major greenhouse gases.
Hella van Asperen, Thorsten Warneke, Alessandro Carioca de Araújo, Bruce Forsberg, Sávio José Filgueiras Ferreira, Thomas Röckmann, Carina van der Veen, Sipko Bulthuis, Leonardo Ramos de Oliveira, Thiago de Lima Xavier, Jailson da Mata, Marta de Oliveira Sá, Paulo Ricardo Teixeira, Julie Andrews de França e Silva, Susan Trumbore, and Justus Notholt
Biogeosciences, 21, 3183–3199, https://doi.org/10.5194/bg-21-3183-2024, https://doi.org/10.5194/bg-21-3183-2024, 2024
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Carbon monoxide (CO) is regarded as an important indirect greenhouse gas. Soils can emit and take up CO, but, until now, uncertainty remains as to which process dominates in tropical rainforests. We present the first soil CO flux measurements from a tropical rainforest. Based on our observations, we report that tropical rainforest soils are a net source of CO. In addition, we show that valley streams and inundated areas are likely additional hot spots of CO in the ecosystem.
Jin Ma, Linda M. J. Kooijmans, Norbert Glatthor, Stephen A. Montzka, Marc von Hobe, Thomas Röckmann, and Maarten C. Krol
Atmos. Chem. Phys., 24, 6047–6070, https://doi.org/10.5194/acp-24-6047-2024, https://doi.org/10.5194/acp-24-6047-2024, 2024
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The global budget of atmospheric COS can be optimised by inverse modelling using TM5-4DVAR, with the co-constraints of NOAA surface observations and MIPAS satellite data. We found reduced COS biosphere uptake from inversions and improved land and ocean separation using MIPAS satellite data assimilation. Further improvements are expected from better quantification of COS ocean and biosphere fluxes.
Katrine A. Gorham, Sam Abernethy, Tyler R. Jones, Peter Hess, Natalie M. Mahowald, Daphne Meidan, Matthew S. Johnson, Maarten M. J. W. van Herpen, Yangyang Xu, Alfonso Saiz-Lopez, Thomas Röckmann, Chloe A. Brashear, Erika Reinhardt, and David Mann
Atmos. Chem. Phys., 24, 5659–5670, https://doi.org/10.5194/acp-24-5659-2024, https://doi.org/10.5194/acp-24-5659-2024, 2024
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Rapid reduction in atmospheric methane is needed to slow the rate of global warming. Reducing anthropogenic methane emissions is a top priority. However, atmospheric methane is also impacted by rising natural emissions and changing sinks. Studies of possible atmospheric methane removal approaches, such as iron salt aerosols to increase the chlorine radical sink, benefit from a roadmapped approach to understand if there may be viable and socially acceptable ways to decrease future risk.
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.
Robbert P. J. Moonen, Getachew A. Adnew, Oscar K. Hartogensis, Jordi Vilà-Guerau de Arellano, David J. Bonell Fontas, and Thomas Röckmann
Atmos. Meas. Tech., 16, 5787–5810, https://doi.org/10.5194/amt-16-5787-2023, https://doi.org/10.5194/amt-16-5787-2023, 2023
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Isotope fluxes allow for net ecosystem gas exchange fluxes to be partitioned into sub-components like plant assimilation, respiration and transpiration, which can help us better understand the environmental drivers of each partial flux. We share the results of a field campaign isotope fluxes were derived using a combination of laser spectroscopy and eddy covariance. We found lag times and high frequency signal loss in the isotope fluxes we derived and present methods to correct for both.
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.
Hossein Maazallahi, Antonio Delre, Charlotte Scheutz, Anders M. Fredenslund, Stefan Schwietzke, Hugo Denier van der Gon, and Thomas Röckmann
Atmos. Meas. Tech., 16, 5051–5073, https://doi.org/10.5194/amt-16-5051-2023, https://doi.org/10.5194/amt-16-5051-2023, 2023
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Measurement methods are increasingly deployed to verify reported methane emissions of gas leaks. This study describes unique advantages and limitations of three methods. Two methods are rapidly deployed, but uncertainties and biases exist for some leak locations. In contrast, the suction method could accurately determine leak rates in principle. However, this method, which provides data for the German emission inventory, creates an overall low bias in our study due to non-random site selection.
Tim René de Groot, Anne Margriet Mol, Katherine Mesdag, Pierre Ramond, Rachel Ndhlovu, Julia Catherine Engelmann, Thomas Röckmann, and Helge Niemann
Biogeosciences, 20, 3857–3872, https://doi.org/10.5194/bg-20-3857-2023, https://doi.org/10.5194/bg-20-3857-2023, 2023
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This study investigates methane dynamics in the Wadden Sea. Our measurements revealed distinct variations triggered by seasonality and tidal forcing. The methane budget was higher in warmer seasons but surprisingly high in colder seasons. Methane dynamics were amplified during low tides, flushing the majority of methane into the North Sea or releasing it to the atmosphere. Methanotrophic activity was also elevated during low tide but mitigated only a small fraction of the methane efflux.
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.
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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Large cities emit greenhouse gases which contribute to global warming. In this study, we measured the release of one important green house gas, methane, in Hamburg. Multiple sources that contribute to methane emissions were located and quantified. Methane sources were found to be mainly caused by human activity (e.g., by release from oil and gas refineries). Moreover, potential natural sources have been located, such as the Elbe River and lakes.
Truls Andersen, Zhao Zhao, Marcel de Vries, Jaroslaw Necki, Justyna Swolkien, Malika Menoud, Thomas Röckmann, Anke Roiger, Andreas Fix, Wouter Peters, and Huilin Chen
Atmos. Chem. Phys., 23, 5191–5216, https://doi.org/10.5194/acp-23-5191-2023, https://doi.org/10.5194/acp-23-5191-2023, 2023
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The Upper Silesian Coal Basin, Poland, is one of the hot spots of methane emissions in Europe. Using an uncrewed aerial vehicle (UAV), we performed atmospheric measurements of methane concentrations downwind of five ventilation shafts in this region and determined the emission rates from the individual shafts. We found a strong correlation between quantified shaft-averaged emission rates and hourly inventory data, which also allows us to estimate the methane emissions from the entire region.
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.
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.
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.
Roland Vernooij, Ulrike Dusek, Maria Elena Popa, Peng Yao, Anupam Shaikat, Chenxi Qiu, Patrik Winiger, Carina van der Veen, Thomas Callum Eames, Natasha Ribeiro, and Guido R. van der Werf
Atmos. Chem. Phys., 22, 2871–2890, https://doi.org/10.5194/acp-22-2871-2022, https://doi.org/10.5194/acp-22-2871-2022, 2022
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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.
Juhi Nagori, Narcisa Nechita-Bândă, Sebastian Oscar Danielache, Masumi Shinkai, Thomas Röckmann, and Maarten Krol
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-68, https://doi.org/10.5194/acp-2022-68, 2022
Publication in ACP not foreseen
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The sulfur isotopes (32S and 34S) were studied to understand the sources, sinks and processes of carbonyl sulphide (COS) in the atmosphere. COS is an important source of sulfur aerosol in the stratosphere (SSA). Few measurements of COS and SSA exist, but with our 1D model, we were able to match them and show the importance of COS to sulfate formation. Moreover, we are able to highlight some important processes for the COS budget and where measurements may fill a gap in current knowledge.
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.
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.
Max Thomas, Johannes C. Laube, Jan Kaiser, Samuel Allin, Patricia Martinerie, Robert Mulvaney, Anna Ridley, Thomas Röckmann, William T. Sturges, and Emmanuel Witrant
Atmos. Chem. Phys., 21, 6857–6873, https://doi.org/10.5194/acp-21-6857-2021, https://doi.org/10.5194/acp-21-6857-2021, 2021
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CFC gases are destroying the Earth's life-protecting ozone layer. We improve understanding of CFC destruction by measuring the isotopic fingerprint of the carbon in the three most abundant CFCs. These are the first such measurements in the main region where CFCs are destroyed – the stratosphere. We reconstruct the atmospheric isotope histories of these CFCs back to the 1950s by measuring air extracted from deep snow and using a model. The model and the measurements are generally consistent.
Hossein Maazallahi, Julianne M. Fernandez, Malika Menoud, Daniel Zavala-Araiza, Zachary D. Weller, Stefan Schwietzke, Joseph C. von Fischer, Hugo Denier van der Gon, and Thomas Röckmann
Atmos. Chem. Phys., 20, 14717–14740, https://doi.org/10.5194/acp-20-14717-2020, https://doi.org/10.5194/acp-20-14717-2020, 2020
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Methane accounts for ∼ 25 % of current climate warming. The current lack of methane measurements is a barrier for tracking major sources, which are key for near-term climate mitigation. We use mobile measurements to identify and quantify methane emission sources in Utrecht (NL) and Hamburg (DE) with a focus on natural gas pipeline leaks. The measurements resulted in fixing the major leaks by the local utility, but coordinated efforts are needed at national levels for further emission reductions.
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.
Alina Fiehn, Julian Kostinek, Maximilian Eckl, Theresa Klausner, Michał Gałkowski, Jinxuan Chen, Christoph Gerbig, Thomas Röckmann, Hossein Maazallahi, Martina Schmidt, Piotr Korbeń, Jarosław Neçki, Pawel Jagoda, Norman Wildmann, Christian Mallaun, Rostyslav Bun, Anna-Leah Nickl, Patrick Jöckel, Andreas Fix, and Anke Roiger
Atmos. Chem. Phys., 20, 12675–12695, https://doi.org/10.5194/acp-20-12675-2020, https://doi.org/10.5194/acp-20-12675-2020, 2020
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A severe reduction of greenhouse gas emissions is necessary to fulfill the Paris Agreement. We use aircraft- and ground-based in situ observations of trace gases and wind speed from two flights over the Upper Silesian Coal Basin, Poland, for independent emission estimation. The derived methane emission estimates are within the range of emission inventories, carbon dioxide estimates are in the lower range and carbon monoxide emission estimates are slightly higher than emission inventory values.
Jordi Vilà-Guerau de Arellano, Patrizia Ney, Oscar Hartogensis, Hugo de Boer, Kevin van Diepen, Dzhaner Emin, Geiske de Groot, Anne Klosterhalfen, Matthias Langensiepen, Maria Matveeva, Gabriela Miranda-García, Arnold F. Moene, Uwe Rascher, Thomas Röckmann, Getachew Adnew, Nicolas Brüggemann, Youri Rothfuss, and Alexander Graf
Biogeosciences, 17, 4375–4404, https://doi.org/10.5194/bg-17-4375-2020, https://doi.org/10.5194/bg-17-4375-2020, 2020
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The CloudRoots field experiment has obtained an open comprehensive observational data set that includes soil, plant, and atmospheric variables to investigate the interactions between a heterogeneous land surface and its overlying atmospheric boundary layer, including the rapid perturbations of clouds in evapotranspiration. Our findings demonstrate that in order to understand and represent diurnal variability, we need to measure and model processes from the leaf to the landscape scales.
Johannes C. Laube, Emma C. Leedham Elvidge, Karina E. Adcock, Bianca Baier, Carl A. M. Brenninkmeijer, Huilin Chen, Elise S. Droste, Jens-Uwe Grooß, Pauli Heikkinen, Andrew J. Hind, Rigel Kivi, Alexander Lojko, Stephen A. Montzka, David E. Oram, Steve Randall, Thomas Röckmann, William T. Sturges, Colm Sweeney, Max Thomas, Elinor Tuffnell, and Felix Ploeger
Atmos. Chem. Phys., 20, 9771–9782, https://doi.org/10.5194/acp-20-9771-2020, https://doi.org/10.5194/acp-20-9771-2020, 2020
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We demonstrate that AirCore technology, which is based on small low-cost balloons, can provide access to trace gas measurements such as CFCs at ultra-low abundances. This is a new way to quantify ozone-depleting, and related, substances in the stratosphere, which is largely inaccessible to aircraft. We show two potential uses: (a) tracking the stratospheric circulation, which is predicted to change, and (b) assessing three common meteorological reanalyses driving a global stratospheric model.
Getachew Agmuas Adnew, Thijs L. Pons, Gerbrand Koren, Wouter Peters, and Thomas Röckmann
Biogeosciences, 17, 3903–3922, https://doi.org/10.5194/bg-17-3903-2020, https://doi.org/10.5194/bg-17-3903-2020, 2020
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We measured the effect of photosynthesis, the largest flux in the carbon cycle, on the triple oxygen isotope composition of atmospheric CO2 at the leaf level during gas exchange using three plant species. The main factors that limit the impact of land vegetation on the triple oxygen isotope composition of atmospheric CO2 are identified, characterized and discussed. The effect of photosynthesis on the isotopic composition of CO2 is commonly quantified as discrimination (ΔA).
Jia Chen, Florian Dietrich, Hossein Maazallahi, Andreas Forstmaier, Dominik Winkler, Magdalena E. G. Hofmann, Hugo Denier van der Gon, and Thomas Röckmann
Atmos. Chem. Phys., 20, 3683–3696, https://doi.org/10.5194/acp-20-3683-2020, https://doi.org/10.5194/acp-20-3683-2020, 2020
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We demonstrate for the first time that large festivals can be significant methane sources, though they are not included in emission inventories. We combined in situ measurements with a Gaussian plume model to determine the Oktoberfest emissions and show that they are not due solely to human biogenic emissions, but are instead primarily fossil fuel related. Our study provides the foundation to develop reduction policies for such events and new pathways to mitigate fossil fuel methane emissions.
Stefan Lossow, Charlotta Högberg, Farahnaz Khosrawi, Gabriele P. Stiller, Ralf Bauer, Kaley A. Walker, Sylvia Kellmann, Andrea Linden, Michael Kiefer, Norbert Glatthor, Thomas von Clarmann, Donal P. Murtagh, Jörg Steinwagner, Thomas Röckmann, and Roland Eichinger
Atmos. Meas. Tech., 13, 287–308, https://doi.org/10.5194/amt-13-287-2020, https://doi.org/10.5194/amt-13-287-2020, 2020
Marco de Bruine, Maarten Krol, Jordi Vilà-Guerau de Arellano, and Thomas Röckmann
Geosci. Model Dev., 12, 5177–5196, https://doi.org/10.5194/gmd-12-5177-2019, https://doi.org/10.5194/gmd-12-5177-2019, 2019
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An aerosol scheme with multiple aerosol species is introduced in the Dutch Atmospheric Large-Eddy Simulation model (DALES) and focused to simulate the feedback of aerosol–cloud interaction (ACI) on the aerosol population. Cloud aerosol processing is found to be sensitive to the numerical method, while removal by precipitation is more stable. How ACI increases or decreases the mean aerosol size depends on the balance between the evaporation of clouds/rain and ultimate removal by precipitation.
Iris N. Dekker, Sander Houweling, Sudhanshu Pandey, Maarten Krol, Thomas Röckmann, Tobias Borsdorff, Jochen Landgraf, and Ilse Aben
Atmos. Chem. Phys., 19, 3433–3445, https://doi.org/10.5194/acp-19-3433-2019, https://doi.org/10.5194/acp-19-3433-2019, 2019
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During November 2017, very high pollution levels were measured in the northern part of India. In this study, satellite (TROPOMI) data and model (WRF) data on carbon monoxide (CO) are studied to investigate the main sources of the CO pollution over the Indo-Gangetic Plain. We found that residential and commercial combustion was a much more important source of CO than the post-monsoon crop burning during this period. Meteorology was found important in the accumulation and ventilation of CO.
Dušan Materić, Elke Ludewig, Kangming Xu, Thomas Röckmann, and Rupert Holzinger
The Cryosphere, 13, 297–307, https://doi.org/10.5194/tc-13-297-2019, https://doi.org/10.5194/tc-13-297-2019, 2019
Marco de Bruine, Maarten Krol, Twan van Noije, Philippe Le Sager, and Thomas Röckmann
Geosci. Model Dev., 11, 1443–1465, https://doi.org/10.5194/gmd-11-1443-2018, https://doi.org/10.5194/gmd-11-1443-2018, 2018
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Precipitation evaporation (PE) and subsequent aerosol resuspension (AR) are currently ignored or implemented only crudely in GCMs. This research introduces PE to Earth system model EC-Earth and explores ways to treat AR and the impact on global aerosol burden. Simple 1:1 scaling of AR with PE leads to an increase (+8 to 15.9 %). Taking into account raindrop size distribution and/or accounting for in-rain aerosol processing decreases aerosol burden -1.5 to 6.2 % and -10 to -11 %, respectively.
Karina E. Adcock, Claire E. Reeves, Lauren J. Gooch, Emma C. Leedham Elvidge, Matthew J. Ashfold, Carl A. M. Brenninkmeijer, Charles Chou, Paul J. Fraser, Ray L. Langenfelds, Norfazrin Mohd Hanif, Simon O'Doherty, David E. Oram, Chang-Feng Ou-Yang, Siew Moi Phang, Azizan Abu Samah, Thomas Röckmann, William T. Sturges, and Johannes C. Laube
Atmos. Chem. Phys., 18, 4737–4751, https://doi.org/10.5194/acp-18-4737-2018, https://doi.org/10.5194/acp-18-4737-2018, 2018
Emma C. Leedham Elvidge, Harald Bönisch, Carl A. M. Brenninkmeijer, Andreas Engel, Paul J. Fraser, Eileen Gallacher, Ray Langenfelds, Jens Mühle, David E. Oram, Eric A. Ray, Anna R. Ridley, Thomas Röckmann, William T. Sturges, Ray F. Weiss, and Johannes C. Laube
Atmos. Chem. Phys., 18, 3369–3385, https://doi.org/10.5194/acp-18-3369-2018, https://doi.org/10.5194/acp-18-3369-2018, 2018
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Chemical species measured in stratospheric air can be used as proxies for stratospheric circulation changes which cannot be measured directly. A range of tracers is important to understand changing stratospheric dynamics. We demonstrate the suitability of PFCs and HFCs as tracers and support recent work that reduces the current stratospheric lifetime of SF6. Updates to policy-relevant parameters (e.g. stratospheric lifetime) linked to this change are provided for O3-depleting substances.
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.
Iris N. Dekker, Sander Houweling, Ilse Aben, Thomas Röckmann, Maarten Krol, Sara Martínez-Alonso, Merritt N. Deeter, and Helen M. Worden
Atmos. Chem. Phys., 17, 14675–14694, https://doi.org/10.5194/acp-17-14675-2017, https://doi.org/10.5194/acp-17-14675-2017, 2017
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This study estimates carbon monoxide emissions from the city of Madrid using MOPITT satellite data. There are two methods used and reviewed in this paper: a method that can only estimate a trend in the emission and a newly developed method that also includes model data from WRF to quantify the emissions. We find Madrid CO emissions to be lower by 48 % for 2002 and by 17 % for 2006 compared with the EdgarV4.2 emission inventory, but uncertainty (20 to 50 %) remains.
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.
Markella Prokopiou, Patricia Martinerie, Célia J. Sapart, Emmanuel Witrant, Guillaume Monteil, Kentaro Ishijima, Sophie Bernard, Jan Kaiser, Ingeborg Levin, Thomas Blunier, David Etheridge, Ed Dlugokencky, Roderik S. W. van de Wal, and Thomas Röckmann
Atmos. Chem. Phys., 17, 4539–4564, https://doi.org/10.5194/acp-17-4539-2017, https://doi.org/10.5194/acp-17-4539-2017, 2017
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Nitrous oxide is the third most important anthropogenic greenhouse gas with an increasing mole fraction. To understand its natural and anthropogenic sources
we employ isotope measurements. Results show that while the N2O mole fraction increases, its heavy isotope content decreases. The isotopic changes observed underline the dominance of agricultural emissions especially at the early part of the record, whereas in the later decades the contribution from other anthropogenic sources increases.
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.
Bastiaan Jonkheid, Thomas Röckmann, Norbert Glatthor, Christof Janssen, Gabriele Stiller, and Thomas von Clarmann
Atmos. Meas. Tech., 9, 6069–6079, https://doi.org/10.5194/amt-9-6069-2016, https://doi.org/10.5194/amt-9-6069-2016, 2016
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.
Matthias Egger, Peter Kraal, Tom Jilbert, Fatimah Sulu-Gambari, Célia J. Sapart, Thomas Röckmann, and Caroline P. Slomp
Biogeosciences, 13, 5333–5355, https://doi.org/10.5194/bg-13-5333-2016, https://doi.org/10.5194/bg-13-5333-2016, 2016
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By combining detailed geochemical analyses with diagenetic modeling, we provide new insights into how methane dynamics may strongly overprint burial records of iron, sulfur and phosphorus in marine systems subject to changes in organic matter loading or water column salinity. A better understanding of these processes will improve our ability to read ancient sediment records and thus to predict the potential consequences of global warming and human-enhanced inputs of nutrients to the ocean.
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.
Sudhanshu Pandey, Sander Houweling, Maarten Krol, Ilse Aben, Frédéric Chevallier, Edward J. Dlugokencky, Luciana V. Gatti, Emanuel Gloor, John B. Miller, Rob Detmers, Toshinobu Machida, and Thomas Röckmann
Atmos. Chem. Phys., 16, 5043–5062, https://doi.org/10.5194/acp-16-5043-2016, https://doi.org/10.5194/acp-16-5043-2016, 2016
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This study investigates the constraint provided by measurements of Xratio (XCH4/XCO2) from space on surface fluxes of CH4 and CO2. We apply the ratio inversion method described in Pandey et al. (2015) to Xratio retrievals from the GOSAT with the TM5-4DVAR inverse modeling system, to constrain the surface fluxes of CH4 and CO2 for 2009 and 2010. The results are compared to proxy CH4 inversions using model-derived-XCO2 mixing ratios from CarbonTracker and MACC.
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.
N. Bândă, M. Krol, M. van Weele, T. van Noije, P. Le Sager, and T. Röckmann
Atmos. Chem. Phys., 16, 195–214, https://doi.org/10.5194/acp-16-195-2016, https://doi.org/10.5194/acp-16-195-2016, 2016
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We quantify the processes responsible for methane growth rate variability in the period 1990 to 1995, a period with variations in climate and radiation due to the Pinatubo eruption. We find significant contributions from changes in the methane emission from wetlands, and in the methane removal by OH caused by stratospheric aerosols, by the decrease in temperature and water vapour, by stratospheric ozone depletion and by changes in emissions of CO and NMVOC.
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.
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.
S. Pandey, S. Houweling, M. Krol, I. Aben, and T. Röckmann
Atmos. Chem. Phys., 15, 8615–8629, https://doi.org/10.5194/acp-15-8615-2015, https://doi.org/10.5194/acp-15-8615-2015, 2015
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This study attempts to determine the feasibility of a new assimilation method of satellite measurements of CH4 and CO2 for optimization of their surface fluxes in a synthetic environment. Instead of their absolute concentrations, we assimilate the ratios of their concentrations (CH4/CO2) in our inversion. Doing so helps us to reduce the effect of atmospheric scattering on the measurements in our system. However, assimilation of the ratios makes the inversion non-linear.
K. Ishijima, M. Takigawa, K. Sudo, S. Toyoda, N. Yoshida, T. Röckmann, J. Kaiser, S. Aoki, S. Morimoto, S. Sugawara, and T. Nakazawa
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-15-19947-2015, https://doi.org/10.5194/acpd-15-19947-2015, 2015
Revised manuscript not accepted
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We developed an atmospheric N2O isotopocule model based on a chemistry-coupled atmospheric general circulation model and a simple method to optimize the model, and estimated the isotopic signatures of surface sources at the hemispheric scale. Data obtained from ground-based observations, measurements of firn air, and balloon and aircraft flights were used to optimize the long-term trends, interhemispheric gradients, and photolytic fractionation, respectively, in the model.
S. J. Allin, J. C. Laube, E. Witrant, J. Kaiser, E. McKenna, P. Dennis, R. Mulvaney, E. Capron, P. Martinerie, T. Röckmann, T. Blunier, J. Schwander, P. J. Fraser, R. L. Langenfelds, and W. T. Sturges
Atmos. Chem. Phys., 15, 6867–6877, https://doi.org/10.5194/acp-15-6867-2015, https://doi.org/10.5194/acp-15-6867-2015, 2015
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Stratospheric ozone protects life on Earth from harmful UV-B radiation. Chlorofluorocarbons (CFCs) are man-made compounds which act to destroy this barrier.
This paper presents (1) the first measurements of the stratospheric δ(37Cl) of CFCs -11 and -113; (2) the first quantification of long-term trends in the tropospheric δ(37Cl) of CFCs -11, -12 and -113.
This study provides a better understanding of source and sink processes associated with these destructive compounds.
F. A. Stap, O. P. Hasekamp, and T. Röckmann
Atmos. Meas. Tech., 8, 1287–1301, https://doi.org/10.5194/amt-8-1287-2015, https://doi.org/10.5194/amt-8-1287-2015, 2015
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We present the capability of an aerosol retrieval algorithm, intended for multi-angle, multi-wavelength photopolarimetric measurements, to intrinsically screen for sub-pixel liquid water cloud contamination.
The screening is based on goodness-of-fit criteria. The algorithm has been applied to a synthetic data set of partially clouded scenes and (non-cloud-screened) POLDER3/PARASOL observations.
S. J. Sutanto, G. Hoffmann, R. A. Scheepmaker, J. Worden, S. Houweling, K. Yoshimura, I. Aben, and T. Röckmann
Atmos. Meas. Tech., 8, 999–1019, https://doi.org/10.5194/amt-8-999-2015, https://doi.org/10.5194/amt-8-999-2015, 2015
D. J. Mrozek, C. van der Veen, M. Kliphuis, J. Kaiser, A. A. Wiegel, and T. Röckmann
Atmos. Meas. Tech., 8, 811–822, https://doi.org/10.5194/amt-8-811-2015, https://doi.org/10.5194/amt-8-811-2015, 2015
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Our analytical system is a promising tool for investigating the triple oxygen isotope composition of CO2 from stratospheric air samples of volumes 100ml and smaller. The method is designed for measuring air samples with CO2 mole fractions between 360 and 400ppm, and it is the first fully automated analytical system that uses CeO2 as the isotope exchange medium.
S. J. Sutanto, B. van den Hurk, P. A. Dirmeyer, S. I. Seneviratne, T. Röckmann, K. E. Trenberth, E. M. Blyth, J. Wenninger, and G. Hoffmann
Hydrol. Earth Syst. Sci., 18, 2815–2827, https://doi.org/10.5194/hess-18-2815-2014, https://doi.org/10.5194/hess-18-2815-2014, 2014
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
A. J. van Beelen, G. J. H. Roelofs, O. P. Hasekamp, J. S. Henzing, and T. Röckmann
Atmos. Chem. Phys., 14, 5969–5987, https://doi.org/10.5194/acp-14-5969-2014, https://doi.org/10.5194/acp-14-5969-2014, 2014
O. Peltola, A. Hensen, C. Helfter, L. Belelli Marchesini, F. C. Bosveld, W. C. M. van den Bulk, J. A. Elbers, S. Haapanala, J. Holst, T. Laurila, A. Lindroth, E. Nemitz, T. Röckmann, A. T. Vermeulen, and I. Mammarella
Biogeosciences, 11, 3163–3186, https://doi.org/10.5194/bg-11-3163-2014, https://doi.org/10.5194/bg-11-3163-2014, 2014
S. Houweling, M. Krol, P. Bergamaschi, C. Frankenberg, E. J. Dlugokencky, I. Morino, J. Notholt, V. Sherlock, D. Wunch, V. Beck, C. Gerbig, H. Chen, E. A. Kort, T. Röckmann, and I. Aben
Atmos. Chem. Phys., 14, 3991–4012, https://doi.org/10.5194/acp-14-3991-2014, https://doi.org/10.5194/acp-14-3991-2014, 2014
B. Ringeval, S. Houweling, P. M. van Bodegom, R. Spahni, R. van Beek, F. Joos, and T. Röckmann
Biogeosciences, 11, 1519–1558, https://doi.org/10.5194/bg-11-1519-2014, https://doi.org/10.5194/bg-11-1519-2014, 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
D. Helmig, V. Petrenko, P. Martinerie, E. Witrant, T. Röckmann, A. Zuiderweg, R. Holzinger, J. Hueber, C. Thompson, J. W. C. White, W. Sturges, A. Baker, T. Blunier, D. Etheridge, M. Rubino, and P. Tans
Atmos. Chem. Phys., 14, 1463–1483, https://doi.org/10.5194/acp-14-1463-2014, https://doi.org/10.5194/acp-14-1463-2014, 2014
F. A. Haumann, A. M. Batenburg, G. Pieterse, C. Gerbig, M. C. Krol, and T. Röckmann
Atmos. Chem. Phys., 13, 9401–9413, https://doi.org/10.5194/acp-13-9401-2013, https://doi.org/10.5194/acp-13-9401-2013, 2013
M. von Hobe, S. Bekki, S. Borrmann, F. Cairo, F. D'Amato, G. Di Donfrancesco, A. Dörnbrack, A. Ebersoldt, M. Ebert, C. Emde, I. Engel, M. Ern, W. Frey, S. Genco, S. Griessbach, J.-U. Grooß, T. Gulde, G. Günther, E. Hösen, L. Hoffmann, V. Homonnai, C. R. Hoyle, I. S. A. Isaksen, D. R. Jackson, I. M. Jánosi, R. L. Jones, K. Kandler, C. Kalicinsky, A. Keil, S. M. Khaykin, F. Khosrawi, R. Kivi, J. Kuttippurath, J. C. Laube, F. Lefèvre, R. Lehmann, S. Ludmann, B. P. Luo, M. Marchand, J. Meyer, V. Mitev, S. Molleker, R. Müller, H. Oelhaf, F. Olschewski, Y. Orsolini, T. Peter, K. Pfeilsticker, C. Piesch, M. C. Pitts, L. R. Poole, F. D. Pope, F. Ravegnani, M. Rex, M. Riese, T. Röckmann, B. Rognerud, A. Roiger, C. Rolf, M. L. Santee, M. Scheibe, C. Schiller, H. Schlager, M. Siciliani de Cumis, N. Sitnikov, O. A. Søvde, R. Spang, N. Spelten, F. Stordal, O. Sumińska-Ebersoldt, A. Ulanovski, J. Ungermann, S. Viciani, C. M. Volk, M. vom Scheidt, P. von der Gathen, K. Walker, T. Wegner, R. Weigel, S. Weinbruch, G. Wetzel, F. G. Wienhold, I. Wohltmann, W. Woiwode, I. A. K. Young, V. Yushkov, B. Zobrist, and F. Stroh
Atmos. Chem. Phys., 13, 9233–9268, https://doi.org/10.5194/acp-13-9233-2013, https://doi.org/10.5194/acp-13-9233-2013, 2013
P. Sperlich, C. Buizert, T. M. Jenk, C. J. Sapart, M. Prokopiou, T. Röckmann, and T. Blunier
Atmos. Meas. Tech., 6, 2027–2041, https://doi.org/10.5194/amt-6-2027-2013, https://doi.org/10.5194/amt-6-2027-2013, 2013
J. Schmitt, B. Seth, M. Bock, C. van der Veen, L. Möller, C. J. Sapart, M. Prokopiou, T. Sowers, T. Röckmann, and H. Fischer
Atmos. Meas. Tech., 6, 1425–1445, https://doi.org/10.5194/amt-6-1425-2013, https://doi.org/10.5194/amt-6-1425-2013, 2013
S. Walter, A. Kock, and T. Röckmann
Biogeosciences, 10, 3391–3403, https://doi.org/10.5194/bg-10-3391-2013, https://doi.org/10.5194/bg-10-3391-2013, 2013
J. C. Laube, A. Keil, H. Bönisch, A. Engel, T. Röckmann, C. M. Volk, and W. T. Sturges
Atmos. Chem. Phys., 13, 2779–2791, https://doi.org/10.5194/acp-13-2779-2013, https://doi.org/10.5194/acp-13-2779-2013, 2013
N. Bândă, M. Krol, M. van Weele, T. van Noije, and T. Röckmann
Atmos. Chem. Phys., 13, 2267–2281, https://doi.org/10.5194/acp-13-2267-2013, https://doi.org/10.5194/acp-13-2267-2013, 2013
Related subject area
Subject: Gases | Technique: Laboratory Measurement | Topic: Instruments and Platforms
Accuracy of tracer-based methane flux quantification: underlying impact of calibrating acetylene measurements
Triple oxygen isotope composition of CO2 in the upper troposphere and stratosphere
Influence of ambient NO and NO2 on the quantification of total peroxy nitrates (ΣPNs) and total alkyl nitrates (ΣANs) by thermal dissociation cavity ring-down spectroscopy (TD-CRDS)
Enhancing forest air sampling using a novel reusable ozone filter design
Identifying key parameters that affect sensitivity of flow tube chemical ionization mass spectrometers
Product ion distributions using H3O+ proton-transfer-reaction time-of-flight mass spectrometry (PTR-ToF-MS): mechanisms, transmission effects, and instrument-to-instrument variability
The Determination of ClNO2 via Thermal Dissociation-Tunable Infrared Laser Direct Absorption Spectroscopy
Simultaneous measurement of greenhouse gases (CH4, CO2 and N2O) using a simplified gas chromatography system
A new portable sampler of atmospheric methane for radiocarbon measurements
High-precision oxygen isotope (δ18O) measurements of atmospheric dioxygen using optical-feedback cavity-enhanced absorption spectroscopy (OF-CEAS)
Water vapor stable isotope memory effects of common tubing materials
Evaluation of a reduced-pressure chemical ion reactor utilizing adduct ionization for the detection of gaseous organic and inorganic species
Ammonium CI-Orbitrap: a tool for characterizing the reactivity of oxygenated organic molecules
A high-accuracy dynamic dilution method for generating reference gas mixtures of carbonyl sulfide at sub-nanomole-per-mole levels for long-term atmospheric observation
Optimizing the iodide-adduct chemical ionization mass spectrometry (CIMS) quantitative method for toluene oxidation intermediates: experimental insights into functional-group differences
Characterization of a new Teflon chamber and on-line analysis of isomeric multifunctional photooxidation products
A versatile water vapor generation module for vapor isotope calibration and liquid isotope measurements
Response of protonated, adduct, and fragmented ions in Vocus proton-transfer-reaction time-of-flight mass spectrometer (PTR-ToF-MS)
Absorption of volatile organic compounds (VOCs) by polymer tubing: implications for indoor air and use as a simple gas-phase volatility separation technique
A flexible device to produce a gas stream with a precisely controlled water vapour mixing ratio and isotope composition based on microdrop dispensing technology
Revision of an open-split-based dual-inlet system for elemental and isotope ratio mass spectrometers with a focus on clumped-isotope measurements
Characterisation of gaseous iodine species detection using the multi-scheme chemical ionisation inlet 2 with bromide and nitrate chemical ionisation methods
A novel inlet for enriching concentrations of reactive organic gases in low sampling flows
Characterizing the automatic radon flux transfer standard system Autoflux: laboratory calibration and field experiments
Influence of ozone and humidity on PTR-MS and GC-MS VOC measurements with and without a Na2S2O3 ozone scrubber
Laser-induced sublimation extraction for centimeter-resolution multi-species greenhouse gas analysis on ice cores
Ozone reactivity measurement of biogenic volatile organic compound emissions
Comparison of two photolytic calibration methods for nitrous acid
Measurement of enantiomer percentages for five monoterpenes from six conifer species by cartridge-tube-based passive sampling adsorption–thermal desorption (ps-ATD)
Identification, monitoring, and reaction kinetics of reactive trace species using time-resolved mid-infrared quantum cascade laser absorption spectroscopy: development, characterisation, and initial results for the CH2OO Criegee intermediate
Air pollution monitoring: development of ammonia (NH3) dynamic reference gas mixtures at nanomoles per mole levels to improve the lack of traceability of measurements
Formaldehyde and glyoxal measurement deploying a selected ion flow tube mass spectrometer (SIFT-MS)
Fragmentation inside proton-transfer-reaction-based mass spectrometers limits the detection of ROOR and ROOH peroxides
MULTICHARME: a modified Chernin-type multi-pass cell designed for IR and THz long-path absorption measurements in the CHARME atmospheric simulation chamber
Silicone tube humidity generator
A source for the continuous generation of pure and quantifiable HONO mixtures
Photochemical method for removing methane interference for improved gas analysis
A simulation chamber for absorption spectroscopy in planetary atmospheres
An automated system for trace gas flux measurements from plant foliage and other plant compartments
Simultaneous measurement of δ13C, δ18O and δ17O of atmospheric CO2 – performance assessment of a dual-laser absorption spectrometer
Measurement of iodine species and sulfuric acid using bromide chemical ionization mass spectrometers
A method for resolving changes in atmospheric He ∕ N2 as an indicator of fossil fuel extraction and stratospheric circulation
Application of chemical derivatization techniques combined with chemical ionization mass spectrometry to detect stabilized Criegee intermediates and peroxy radicals in the gas phase
Atomic emission detector with gas chromatographic separation and cryogenic pre-concentration (CryoTrap–GC–AED) for atmospheric trace gas measurements
New technique for high-precision, simultaneous measurements of CH4, N2O and CO2 concentrations; isotopic and elemental ratios of N2, O2 and Ar; and total air content in ice cores by wet extraction
High-precision laser spectrometer for multiple greenhouse gas analysis in 1 mL air from ice core samples
A thermal-dissociation–cavity ring-down spectrometer (TD-CRDS) for the detection of organic nitrates in gas and particle phases
Interference from alkenes in chemiluminescent NOx measurements
Calibration of an airborne HOx instrument using the All Pressure Altitude-based Calibrator for HOx Experimentation (APACHE)
Measurement of ammonia, amines and iodine compounds using protonated water cluster chemical ionization mass spectrometry
Adil Shah, Olivier Laurent, Pramod Kumar, Grégoire Broquet, Loïc Loigerot, Timothé Depelchin, Mathis Lozano, Camille Yver Kwok, Carole Philippon, Clément Romand, Elisa Allegrini, Matthieu Trombetti, and Philippe Ciais
Atmos. Meas. Tech., 18, 3425–3451, https://doi.org/10.5194/amt-18-3425-2025, https://doi.org/10.5194/amt-18-3425-2025, 2025
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Acetylene mole fraction measurements from the Picarro G2203 were characterised. Abnormal sensor behaviour was observed in wet conditions. A dry linear calibration was derived, although this was invalid below 1.2 ppb due to unstable measurements. The instrument was used to measure acetylene as a methane tracer at a landfill site. Fluxes were derived from 14 downwind transects using both raw and calibrated acetylene mole fraction, with raw measurements resulting in 8 % flux underestimation.
Getachew Agmuas Adnew, Gerbrand Koren, Neha Mehendale, Sergey Gromov, Maarten Krol, and Thomas Röckmann
Atmos. Meas. Tech., 18, 2701–2719, https://doi.org/10.5194/amt-18-2701-2025, https://doi.org/10.5194/amt-18-2701-2025, 2025
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This study presents high-precision measurements of ∆′17O(CO2). Key findings include the extension of the N2O–∆′17O correlation to the upper troposphere and the identification of significant differences in the N2O–∆′17O slope in StratoClim samples. Additionally, the ∆′17O measurements are used to estimate global stratospheric production and surface removal of ∆′17O, providing an independent estimate of global vegetation CO2 exchange.
Laura Wüst, Patrick Dewald, Gunther N. T. E. Türk, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 18, 1943–1959, https://doi.org/10.5194/amt-18-1943-2025, https://doi.org/10.5194/amt-18-1943-2025, 2025
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Detection of NO2 via cavity ring-down spectroscopy (CRDS) after thermal dissociation (TD) of alkyl and peroxy nitrates can be used to detect total atmospheric organic nitrates originating from the interaction between biogenic emissions of volatile organic compounds and nitrogen oxides of anthropogenic origin. Here we present an improved TD-CRDS technique that avoids systematic bias resulting from secondary chemistry in the heated inlets and that can be deployed in regions with strong biogenic emissions.
Robby Rynek, Thomas Mayer, and Helko Borsdorf
EGUsphere, https://doi.org/10.5194/egusphere-2025-1387, https://doi.org/10.5194/egusphere-2025-1387, 2025
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A novel, reusable ozone filter design for the monitoring of biogenic volatile organic compounds using sorbent tubes and multi-tube samplers was evaluated. The ozone filters proved high efficiency in retaining high recovery rates across different environmental relevant levels of relative humidity and ozone concentrations, while safeguarding the sorbent material, both in laboratory and field experiments. The filter design has the advantage of not requiring additional equipment or regular checks.
Sneha Aggarwal, Priyanka Bansal, Yuwei Wang, Spiro Jorga, Gabrielle Macgregor, Urs Rohner, Thomas Bannan, Matthew Salter, Paul Zieger, Claudia Mohr, and Felipe Lopez-Hilfiker
EGUsphere, https://doi.org/10.5194/egusphere-2025-696, https://doi.org/10.5194/egusphere-2025-696, 2025
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Chemical ionization mass spectrometers used for trace gas analysis can be operated at various conditions, complicating quantitative comparisons. We evaluate sensitivity dependence on relatively few key instrument parameters and show that when these are held constant, consistent performance is achieved. We show that the maximum sensitivity of a given flow tube reactor across various reagent ion chemistries is a constant, which aids in the quantification of compounds lacking analytical standards.
Michael F. Link, Megan S. Claflin, Christina E. Cecelski, Ayomide A. Akande, Delaney Kilgour, Paul A. Heine, Matthew Coggon, Chelsea E. Stockwell, Andrew Jensen, Jie Yu, Han N. Huynh, Jenna C. Ditto, Carsten Warneke, William Dresser, Keighan Gemmell, Spiro Jorga, Rileigh L. Robertson, Joost de Gouw, Timothy Bertram, Jonathan P. D. Abbatt, Nadine Borduas-Dedekind, and Dustin Poppendieck
Atmos. Meas. Tech., 18, 1013–1038, https://doi.org/10.5194/amt-18-1013-2025, https://doi.org/10.5194/amt-18-1013-2025, 2025
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Proton-transfer-reaction mass spectrometry (PTR-MS) is widely used for the measurement of volatile organic compounds (VOCs) both indoors and outdoors. An analytical challenge for PTR-MS measurements is the formation of unintended measurement interferences, product ion distributions (PIDs), that may appear in the data as VOCs of interest. We developed a method for quantifying PID formation and use interlaboratory comparison data to put quantitative constraints on PID formation.
John W. Halfacre, Lewis Marden, Marvin D. Shaw, Lucy J. Carpenter, Emily Matthews, Thomas J. Bannan, Hugh Coe, Scott C. Herndon, Joseph R. Roscioli, Christoph Dyroff, Tara I. Yacovitch, Patrick R. Veres, Michael A. Robinson, Steven S. Brown, and Pete M. Edwards
EGUsphere, https://doi.org/10.5194/egusphere-2025-831, https://doi.org/10.5194/egusphere-2025-831, 2025
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Nitryl chloride (ClNO2) is a reservoir of chlorine atoms and nitrogen oxides, both of which play important roles in atmospheric chemistry. However, all ambient ClNO2 observations so far have been made by a single technique, mass spectrometry, which needs complex calibrations. Here, we present a laser-based method that detects ClNO2 (TD-TILDAS) without the need for complicated calibrations. The results show excellent agreement between these two methods from both laboratory and ambient samples.
Michał Bucha, Dominika Lewicka-Szczebak, and Piotr Wójtowicz
Atmos. Meas. Tech., 18, 897–908, https://doi.org/10.5194/amt-18-897-2025, https://doi.org/10.5194/amt-18-897-2025, 2025
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We present a method for the determination of greenhouse gases (CH4, CO2, N2O) using a chromatographic system with a barrier ion discharge detector (BID) and a Carboxen 1010 capillary column. The system omits the need for an electron capture detector (ECD) containing radiogenic components for N2O analysis and a flame ionisation detector (FID) with a methaniser for CO2 samples. This simplification reduces analytical costs, facilitates instrument maintenance and improves measurement robustness.
Giulia Zazzeri, Lukas Wacker, Negar Haghipour, Philip Gautschi, Thomas Laemmel, Sönke Szidat, and Heather Graven
Atmos. Meas. Tech., 18, 319–325, https://doi.org/10.5194/amt-18-319-2025, https://doi.org/10.5194/amt-18-319-2025, 2025
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Radiocarbon (14C) is an optimal tracer of methane (CH4) emissions, as 14C measurements enable distinguishing between fossil methane and biogenic methane. However, these measurements are particularly challenging, mainly due to technical difficulties in the sampling procedure. We made the sample extraction much simpler and time efficient, providing a new technology that can be used by any research group, with the goal of expanding 14C measurements for an improved understanding of methane sources.
Clément Piel, Daniele Romanini, Morgane Farradèche, Justin Chaillot, Clémence Paul, Nicolas Bienville, Thomas Lauwers, Joana Sauze, Kévin Jaulin, Frédéric Prié, and Amaëlle Landais
Atmos. Meas. Tech., 17, 6647–6658, https://doi.org/10.5194/amt-17-6647-2024, https://doi.org/10.5194/amt-17-6647-2024, 2024
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This paper introduces a new optical gas analyzer based on an optical-feedback cavity-enhanced absorption spectroscopy (OF-CEAS) technique enabling high-temporal-resolution and high-precision measurements of oxygen isotopes (δ18O) and dioxygen (O2) concentration of atmospheric O2 (respectively 0.06 ‰ and 0.002 % over 10 min integration). The results underscore the good agreement with isotope ratio mass spectrometry measurements and the ability of the instrument to monitor biological processes.
Alexandra L. Meyer and Lisa R. Welp
Atmos. Meas. Tech., 17, 6193–6212, https://doi.org/10.5194/amt-17-6193-2024, https://doi.org/10.5194/amt-17-6193-2024, 2024
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Water molecules stick to air intake tubing wall surfaces, smoothing measurements of fast isotopic variability in the atmosphere. We tested this stickiness and saw small differences in isotopic signal speed between materials, tubing inner dimensions, and isotopic switch direction, although no consistent temperature effects. Researchers can confidently compare measurements across observation systems using different commonly used tubing materials and plan for optimal inlet designs of new systems.
Matthieu Riva, Veronika Pospisilova, Carla Frege, Sebastien Perrier, Priyanka Bansal, Spiro Jorga, Patrick Sturm, Joel A. Thornton, Urs Rohner, and Felipe Lopez-Hilfiker
Atmos. Meas. Tech., 17, 5887–5901, https://doi.org/10.5194/amt-17-5887-2024, https://doi.org/10.5194/amt-17-5887-2024, 2024
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We present a newly designed reduced-pressure chemical ionization reactor for detection of gas-phase organic and inorganic species. The system operates through the combined use of vacuum ultraviolet ionization and photosensitizers to generate numerous adduct ionization schemes. As a result, it offers the ability to simultaneously measure a wide variety of organic and inorganic species in terms of compound volatility and functionality, while being largely independent of changes in sample humidity.
Dandan Li, Dongyu Wang, Lucia Caudillo, Wiebke Scholz, Mingyi Wang, Sophie Tomaz, Guillaume Marie, Mihnea Surdu, Elias Eccli, Xianda Gong, Loic Gonzalez-Carracedo, Manuel Granzin, Joschka Pfeifer, Birte Rörup, Benjamin Schulze, Pekka Rantala, Sébastien Perrier, Armin Hansel, Joachim Curtius, Jasper Kirkby, Neil M. Donahue, Christian George, Imad El-Haddad, and Matthieu Riva
Atmos. Meas. Tech., 17, 5413–5428, https://doi.org/10.5194/amt-17-5413-2024, https://doi.org/10.5194/amt-17-5413-2024, 2024
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Due to the analytical challenges of measuring organic vapors, it remains challenging to identify and quantify organic molecules present in the atmosphere. Here, we explore the performance of the Orbitrap chemical ionization mass spectrometer (CI-Orbitrap) using ammonium ion chemistry. This study shows that ammonium-ion-based chemistry associated with the high mass resolution of the Orbitrap mass analyzer can measure almost all inclusive compounds.
Hideki Nara, Takuya Saito, Taku Umezawa, and Yasunori Tohjima
Atmos. Meas. Tech., 17, 5187–5200, https://doi.org/10.5194/amt-17-5187-2024, https://doi.org/10.5194/amt-17-5187-2024, 2024
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We have developed a high-accuracy dynamic dilution system for generating reference gas mixtures containing carbonyl sulfide (COS). Although COS at ambient levels generally has poor storage stability, our approach involves the dilution of a gas mixture containing micromole-per-mole levels of COS, the stability of which was validated for more than 1 decade. The developed system has excellent dilution performance and will facilitate accurate instrumental calibration for atmospheric COS observation.
Mengdi Song, Shuyu He, Xin Li, Ying Liu, Shengrong Lou, Sihua Lu, Limin Zeng, and Yuanhang Zhang
Atmos. Meas. Tech., 17, 5113–5127, https://doi.org/10.5194/amt-17-5113-2024, https://doi.org/10.5194/amt-17-5113-2024, 2024
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We introduce detailed and improved quantitation and semi-quantitation methods of iodide-adduct time-of-flight chemical ionization mass spectrometry (I-CIMS) to measure toluene oxidation intermediates. We assess the experimental sensitivity of various functional group species and their binding energy with iodide ions in I-CIMS. A novel classification approach was introduced to significantly enhance the accuracy of semi-quantitative methods (improving R2 values from 0.52 to beyond 0.88).
Finja Löher, Esther Borrás, Amalia Muñoz, and Anke Christine Nölscher
Atmos. Meas. Tech., 17, 4553–4579, https://doi.org/10.5194/amt-17-4553-2024, https://doi.org/10.5194/amt-17-4553-2024, 2024
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We constructed and characterized a new indoor Teflon atmospheric simulation chamber. We evaluated wall losses, photolysis rates, and secondary reactions of multifunctional photooxidation products in the chamber. To measure these products on-line, we combined chromatographic and mass spectrometric analyses to obtain both isomeric information and a high temporal resolution. For method validation, we studied the formation yields of the main ring-retaining products of toluene.
Hans Christian Steen-Larsen and Daniele Zannoni
Atmos. Meas. Tech., 17, 4391–4409, https://doi.org/10.5194/amt-17-4391-2024, https://doi.org/10.5194/amt-17-4391-2024, 2024
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The water vapor generation module is completely scalable, allowing autonomous calibrations to use N standards and providing integration times only restricted by sample availability. We document improved reproducibility in 17O-excess liquid measurements. This module makes spectroscopy measurements comparable to mass spectrometry. We document that the vapor generation module can be used to analyze instrument performance and for vapor isotope calibration during field campaign measurements.
Fangbing Li, Dan Dan Huang, Linhui Tian, Bin Yuan, Wen Tan, Liang Zhu, Penglin Ye, Douglas Worsnop, Ka In Hoi, Kai Meng Mok, and Yong Jie Li
Atmos. Meas. Tech., 17, 2415–2427, https://doi.org/10.5194/amt-17-2415-2024, https://doi.org/10.5194/amt-17-2415-2024, 2024
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The responses of protonated, adduct, and fragmented ions of 21 volatile organic compounds (VOCs) were investigated with varying instrument settings and relative humidity (RH) in a Vocus proton-transfer-reaction mass spectrometer (PTR-MS). The protonated ions of most VOCs studied show < 15 % variation in sensitivity, except for some long-chain aldehydes. The relationship between sensitivity and PTR rate constant is complicated by the influences from ion transmission and protonated ion fraction.
Melissa A. Morris, Demetrios Pagonis, Douglas A. Day, Joost A. de Gouw, Paul J. Ziemann, and Jose L. Jimenez
Atmos. Meas. Tech., 17, 1545–1559, https://doi.org/10.5194/amt-17-1545-2024, https://doi.org/10.5194/amt-17-1545-2024, 2024
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Polymer absorption of volatile organic compounds (VOCs) is important to characterize for atmospheric sampling setups (as interactions cause sampling delays) and indoor air quality. Here we test different polymer materials and quantify their absorptive capacities through modeling. We found the main polymers in carpets to be highly absorptive, acting as large reservoirs for indoor pollution. We also demonstrated how polymer tubes can be used as a low-cost gas separation technique.
Harald Sodemann, Alena Dekhtyareva, Alvaro Fernandez, Andrew Seidl, and Jenny Maccali
Atmos. Meas. Tech., 16, 5181–5203, https://doi.org/10.5194/amt-16-5181-2023, https://doi.org/10.5194/amt-16-5181-2023, 2023
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We describe a device that allows one to produce a continuous stream of water vapour with a specified level of humidity. As a main innovation, we can mix waters with different water isotope composition. Through a series of tests we show that the performance characteristics of the device are in line with specifications. We present two laboratory applications where the device proves useful, first in characterizing instruments, and second for the analysis of water contained in stalagmites.
Stephan Räss, Peter Nyfeler, Paul Wheeler, Will Price, and Markus Christian Leuenberger
Atmos. Meas. Tech., 16, 4489–4505, https://doi.org/10.5194/amt-16-4489-2023, https://doi.org/10.5194/amt-16-4489-2023, 2023
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Due to technological advances clumped-isotope studies have gained importance in recent years. Typically, these studies are performed with high-resolution isotope ratio mass spectrometers (IRMSs) along with a changeover-valve-based dual-inlet system (DIS). We are taking a different approach, namely performing clumped-isotope measurements with a compact low-resolution IRMS with an open-split-based DIS. Currently, we are working with pure-oxygen gas for which we are providing a proof of concept.
Xu-Cheng He, Jiali Shen, Siddharth Iyer, Paxton Juuti, Jiangyi Zhang, Mrisha Koirala, Mikko M. Kytökari, Douglas R. Worsnop, Matti Rissanen, Markku Kulmala, Norbert M. Maier, Jyri Mikkilä, Mikko Sipilä, and Juha Kangasluoma
Atmos. Meas. Tech., 16, 4461–4487, https://doi.org/10.5194/amt-16-4461-2023, https://doi.org/10.5194/amt-16-4461-2023, 2023
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In this study, the upgraded multi-scheme chemical ionisation inlet 2 is presented. Sulfuric acid, hypoiodous acid, iodine, sulfur dioxide, and hydroperoxyl radicals are calibrated, and the improved ion optics allow us to detect sulfuric acid and iodine-containing molecules at as low as a few parts per quadrillion by volume. Additionally, we confirm the reliable detection of iodic acid using both the nitrate and bromide chemical ionisation methods under atmospherically relevant conditions.
Namrata Shanmukh Panji and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 16, 4319–4330, https://doi.org/10.5194/amt-16-4319-2023, https://doi.org/10.5194/amt-16-4319-2023, 2023
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Measuring volatile organic compounds (VOCs) in the atmosphere is crucial for understanding air quality and environmental impact. Since these compounds are present in low concentrations, preconcentration of samples is often necessary for accurate detection. To address this issue, we have developed a novel inlet that uses selective permeation to concentrate organic gases in small sample flows. This device offers a promising approach for accurately detecting low levels of VOCs in the atmosphere.
Claudia Grossi, Daniel Rabago, Scott Chambers, Carlos Sáinz, Roger Curcoll, Peter P. S. Otáhal, Eliška Fialová, Luis Quindos, and Arturo Vargas
Atmos. Meas. Tech., 16, 2655–2672, https://doi.org/10.5194/amt-16-2655-2023, https://doi.org/10.5194/amt-16-2655-2023, 2023
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The automatic and low-maintenance radon flux system Autoflux, completed with environmental soil and atmosphere sensors, has been theoretically and experimentally characterized and calibrated under laboratory conditions to be used as transfer standard for in situ measurements. It will offer for the first time long-term measurements to validate radon flux maps used by the climate and the radiation protection communities for assessing the radon gas emissions in the atmosphere.
Lisa Ernle, Monika Akima Ringsdorf, and Jonathan Williams
Atmos. Meas. Tech., 16, 1179–1194, https://doi.org/10.5194/amt-16-1179-2023, https://doi.org/10.5194/amt-16-1179-2023, 2023
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Atmospheric ozone can induce artefacts in volatile organic compound measurements. Laboratory tests were made using GC-MS and PTR-MS aircraft systems under tropospheric and stratospheric conditions of humidity and ozone, with and without sodium thiosulfate filter scrubbers. Ozone in dry air produces some carbonyls and degrades alkenes. The scrubber lifetime depends on ozone concentration, flow rate and humidity. For the troposphere with scrubber, no significant artefacts were found over 14 d.
Lars Mächler, Daniel Baggenstos, Florian Krauss, Jochen Schmitt, Bernhard Bereiter, Remo Walther, Christoph Reinhard, Béla Tuzson, Lukas Emmenegger, and Hubertus Fischer
Atmos. Meas. Tech., 16, 355–372, https://doi.org/10.5194/amt-16-355-2023, https://doi.org/10.5194/amt-16-355-2023, 2023
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We present a new method to extract the gases from ice cores and measure their greenhouse gas composition. The ice is sublimated continuously with a near-infrared laser, releasing the gases, which are then analyzed on a laser absorption spectrometer. The main advantage over previous efforts is a low effective resolution of 1–2 cm. This capability is crucial for the analysis of highly thinned ice, as expected from ongoing drilling efforts to extend ice core history further back in time.
Detlev Helmig, Alex Guenther, Jacques Hueber, Ryan Daly, Wei Wang, Jeong-Hoo Park, Anssi Liikanen, and Arnaud P. Praplan
Atmos. Meas. Tech., 15, 5439–5454, https://doi.org/10.5194/amt-15-5439-2022, https://doi.org/10.5194/amt-15-5439-2022, 2022
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This research demonstrates a new method for determination of the chemical reactivity of volatile organic compounds that are emitted from the leaves and needles of trees. These measurements allow elucidating if and how much of these emissions and their associated reactivity are captured and quantified by currently applicable chemical analysis methods.
Andrew J. Lindsay and Ezra C. Wood
Atmos. Meas. Tech., 15, 5455–5464, https://doi.org/10.5194/amt-15-5455-2022, https://doi.org/10.5194/amt-15-5455-2022, 2022
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Nitrous acid (HONO) is an important source of the main atmospheric oxidant – the hydroxyl radical (OH). Advances in nitrous acid measurement techniques and calibration methods therefore improve our understanding of atmospheric oxidation processes. In this paper, we present two calibration methods based on photo-dissociating water vapor. These calibration methods are useful alternatives to conventional calibrations that involve a reacting hydrogen chloride vapor with sodium nitrite.
Ying Wang, Wentai Luo, Todd N. Rosenstiel, and James F. Pankow
Atmos. Meas. Tech., 15, 4651–4661, https://doi.org/10.5194/amt-15-4651-2022, https://doi.org/10.5194/amt-15-4651-2022, 2022
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A rapid, sensitive, and precise analytical method was developed for measuring the fractional amounts of the (−) and (+) forms of chiral enantiomeric forms of monoterpenes in air containing biogenic plant emissions. The method uses passive air sampling onto adsorption–thermal desorption (ATD) gas sampling cartridge tubes; this is followed by automatable thermal desorption onto a chiral gas chromatography (GC) column, followed by detection with mass spectrometry (MS).
Zara S. Mir, Matthew Jamieson, Nicholas R. Greenall, Paul W. Seakins, Mark A. Blitz, and Daniel Stone
Atmos. Meas. Tech., 15, 2875–2887, https://doi.org/10.5194/amt-15-2875-2022, https://doi.org/10.5194/amt-15-2875-2022, 2022
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In this work we describe the development and characterisation of an experiment using laser flash photolysis coupled with time-resolved mid-infrared (mid-IR) quantum cascade laser (QCL) absorption spectroscopy, with initial results reported for measurements of the infrared spectrum, kinetics, and product yields for the reaction of the CH2OO Criegee intermediate with SO2. This work has significance for the identification and measurement of reactive trace species in complex systems.
Tatiana Macé, Maitane Iturrate-Garcia, Céline Pascale, Bernhard Niederhauser, Sophie Vaslin-Reimann, and Christophe Sutour
Atmos. Meas. Tech., 15, 2703–2718, https://doi.org/10.5194/amt-15-2703-2022, https://doi.org/10.5194/amt-15-2703-2022, 2022
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LNE developed, with the company 2M PROCESS, a gas reference generator to dynamically generate NH3 reference gas mixtures in the air at very low fractions between 1 and 400 nmol/mol. The procedure defined by LNE for calibrating NH3 analyzers used for monitoring air quality guarantees relative expanded uncertainties lower than 2 % for this measurement range. The results of a comparison organized between METAS and LNE allowed the validation of LNE's reference generator and calibration procedure.
Antonia G. Zogka, Manolis N. Romanias, and Frederic Thevenet
Atmos. Meas. Tech., 15, 2001–2019, https://doi.org/10.5194/amt-15-2001-2022, https://doi.org/10.5194/amt-15-2001-2022, 2022
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We emphasize the application of SIFT-MS to detect two important atmospheric pollutants, i.e., formaldehyde (FM) and glyoxal (GL). FM and GL are secondary products formed by volatile organic compound oxidation in indoor and outdoor environments and play a key role in air quality and climate. We show that SIFT-MS is able to monitor these species selectively and in real time, overcoming the limitations of other, classical analytical techniques used to monitor these species in the atmosphere.
Haiyan Li, Thomas Golin Almeida, Yuanyuan Luo, Jian Zhao, Brett B. Palm, Christopher D. Daub, Wei Huang, Claudia Mohr, Jordan E. Krechmer, Theo Kurtén, and Mikael Ehn
Atmos. Meas. Tech., 15, 1811–1827, https://doi.org/10.5194/amt-15-1811-2022, https://doi.org/10.5194/amt-15-1811-2022, 2022
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This work evaluated the potential for PTR-based mass spectrometers to detect ROOR and ROOH peroxides both experimentally and through computations. Laboratory experiments using a Vocus PTR observed only noisy signals of potential dimers during α-pinene ozonolysis and a few small signals of dimeric compounds during cyclohexene ozonolysis. Quantum chemical calculations for model ROOR and ROOH systems showed that most of these peroxides should fragment partially following protonation.
Jean Decker, Éric Fertein, Jonas Bruckhuisen, Nicolas Houzel, Pierre Kulinski, Bo Fang, Weixiong Zhao, Francis Hindle, Guillaume Dhont, Robin Bocquet, Gaël Mouret, Cécile Coeur, and Arnaud Cuisset
Atmos. Meas. Tech., 15, 1201–1215, https://doi.org/10.5194/amt-15-1201-2022, https://doi.org/10.5194/amt-15-1201-2022, 2022
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We present a multiple pass system developed for the CHamber for Atmospheric Reactivity and Metrology of the Environment. This multi-pass cell allows monitoring of atmospheric species at trace levels by high-resolution spectroscopy with long interaction path lengths in the IR and for the first time in the terahertz range. Interesting prospects are highlighted in this frequency domain, such as a high degree of selectivity or the possibility to monitor in real-time atmospheric processes.
Robert F. Berg, Nicola Chiodo, and Eric Georgin
Atmos. Meas. Tech., 15, 819–832, https://doi.org/10.5194/amt-15-819-2022, https://doi.org/10.5194/amt-15-819-2022, 2022
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We made a humidity generator that adds water vapor to a flowing gas. Its range of humidity is useful for calibrating balloon-borne probes to the Earth's stratosphere. The generator’s novel feature is a saturator that comprises 5 m of silicone tubing immersed in water. The length was enough to ensure that the saturator’s output was independent of the dimensions and permeability of the tube. This simple, low-cost design provides an accuracy that is acceptable for many applications.
Guillermo Villena and Jörg Kleffmann
Atmos. Meas. Tech., 15, 627–637, https://doi.org/10.5194/amt-15-627-2022, https://doi.org/10.5194/amt-15-627-2022, 2022
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A continuous source for the generation of pure HONO mixtures was developed and characterized, which is based on the Henry's law solubility of HONO in acidic aqueous solutions. The source shows a fast time response and an excellent long-term stability and can be easily adjusted to HONO mixing ratios in the range 0.05–500 ppb. A general equation based on Henry's law is developed, whereby the HONO concentration of the source can be absolutely calculated with an accuracy of better than 10 %.
Merve Polat, Jesper Baldtzer Liisberg, Morten Krogsbøll, Thomas Blunier, and Matthew S. Johnson
Atmos. Meas. Tech., 14, 8041–8067, https://doi.org/10.5194/amt-14-8041-2021, https://doi.org/10.5194/amt-14-8041-2021, 2021
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We have designed a process for removing methane from a gas stream so that nitrous oxide can be measured without interference. These are both key long-lived greenhouse gases frequently studied in relation to ice cores, plants, water treatment and so on. However, many researchers are not aware of the problem of methane interference, and in addition there have not been good methods available for solving the problem. Here we present and evaluate such a method.
Marcel Snels, Stefania Stefani, Angelo Boccaccini, David Biondi, and Giuseppe Piccioni
Atmos. Meas. Tech., 14, 7187–7197, https://doi.org/10.5194/amt-14-7187-2021, https://doi.org/10.5194/amt-14-7187-2021, 2021
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A novel simulation chamber, PASSxS (Planetary Atmosphere Simulation System for Spectroscopy), has been developed for absorption measurements with a Fourier transform spectrometer (FTS) and possibly a cavity ring-down (CRD) spectrometer, with a sample temperature ranging from 100 K up to 550 K, while the pressure of the gas can be varied up to 60 bar. These temperature and pressure ranges cover a significant part of the planetary atmospheres in the solar system and possibly extrasolar planets.
Lukas Kohl, Markku Koskinen, Tatu Polvinen, Salla Tenhovirta, Kaisa Rissanen, Marjo Patama, Alessandro Zanetti, and Mari Pihlatie
Atmos. Meas. Tech., 14, 4445–4460, https://doi.org/10.5194/amt-14-4445-2021, https://doi.org/10.5194/amt-14-4445-2021, 2021
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We present ShoTGa-FluMS, a measurement system designed for continuous and automated measurements of trace gas and volatile organic compound (VOC) fluxes from plant shoots. ShoTGa-FluMS uses transparent shoot enclosures equipped with cooling elements, automatically replaces fixated CO2, and removes transpired water from the enclosure, thus solving multiple technical problems that have so far prevented automated plant shoot trace gas flux measurements.
Pharahilda M. Steur, Hubertus A. Scheeren, Dave D. Nelson, J. Barry McManus, and Harro A. J. Meijer
Atmos. Meas. Tech., 14, 4279–4304, https://doi.org/10.5194/amt-14-4279-2021, https://doi.org/10.5194/amt-14-4279-2021, 2021
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For understanding the sources and sinks of atmospheric CO2, measurement of stable isotopes has proven to be highly valuable. We present a new method using laser absorption spectroscopy to simultaneously conduct measurements of three CO2 isotopes, directly on dry-air samples. This new method reduces sample preparation time significantly, compared to the conventional method in which measurements are conducted on pure CO2, and avoids measurement biases introduced by CO2 extraction.
Mingyi Wang, Xu-Cheng He, Henning Finkenzeller, Siddharth Iyer, Dexian Chen, Jiali Shen, Mario Simon, Victoria Hofbauer, Jasper Kirkby, Joachim Curtius, Norbert Maier, Theo Kurtén, Douglas R. Worsnop, Markku Kulmala, Matti Rissanen, Rainer Volkamer, Yee Jun Tham, Neil M. Donahue, and Mikko Sipilä
Atmos. Meas. Tech., 14, 4187–4202, https://doi.org/10.5194/amt-14-4187-2021, https://doi.org/10.5194/amt-14-4187-2021, 2021
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Atmospheric iodine species are often short-lived with low abundance and have thus been challenging to measure. We show that the bromide chemical ionization mass spectrometry, compatible with both the atmospheric pressure and reduced pressure interfaces, can simultaneously detect various gas-phase iodine species. Combining calibration experiments and quantum chemical calculations, we quantify detection sensitivities to HOI, HIO3, I2, and H2SO4, giving detection limits down to < 106 molec. cm-3.
Benjamin Birner, William Paplawsky, Jeffrey Severinghaus, and Ralph F. Keeling
Atmos. Meas. Tech., 14, 2515–2527, https://doi.org/10.5194/amt-14-2515-2021, https://doi.org/10.5194/amt-14-2515-2021, 2021
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The atmospheric helium-to-nitrogen ratio is a promising indicator for circulation changes in the upper atmosphere and fossil fuel burning by humans. We present a very precise analysis method to determine changes in the helium-to-nitrogen ratio of air samples. The method relies on stabilizing the gas flow to a mass spectrometer and continuous removal of reactive gases. These advances enable new insights and monitoring possibilities for anthropogenic and natural processes.
Alexander Zaytsev, Martin Breitenlechner, Anna Novelli, Hendrik Fuchs, Daniel A. Knopf, Jesse H. Kroll, and Frank N. Keutsch
Atmos. Meas. Tech., 14, 2501–2513, https://doi.org/10.5194/amt-14-2501-2021, https://doi.org/10.5194/amt-14-2501-2021, 2021
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We have developed an online method for speciated measurements of organic peroxy radicals and stabilized Criegee intermediates using chemical derivatization combined with chemical ionization mass spectrometry. Chemical derivatization prevents secondary radical reactions and eliminates potential interferences. Comparison between our measurements and results from numeric modeling shows that the method can be used for the quantification of a wide range of atmospheric radicals and intermediates.
Einar Karu, Mengze Li, Lisa Ernle, Carl A. M. Brenninkmeijer, Jos Lelieveld, and Jonathan Williams
Atmos. Meas. Tech., 14, 1817–1831, https://doi.org/10.5194/amt-14-1817-2021, https://doi.org/10.5194/amt-14-1817-2021, 2021
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A gas measurement device was developed to measure trace gases (ppt level) in the air based on an atomic emission detector. It combines a cryogenic pre-concentrator (CryoTrap), a gas chromatograph (GC), and a new high-resolution atomic emission detector (AED). The CryoTrap–GC–AED instrumental setup, limits of detection, and elemental performance are presented and discussed. Two measurement case studies are reported: one in a Finnish boreal forest and the other based on an aircraft campaign.
Ikumi Oyabu, Kenji Kawamura, Kyotaro Kitamura, Remi Dallmayr, Akihiro Kitamura, Chikako Sawada, Jeffrey P. Severinghaus, Ross Beaudette, Anaïs Orsi, Satoshi Sugawara, Shigeyuki Ishidoya, Dorthe Dahl-Jensen, Kumiko Goto-Azuma, Shuji Aoki, and Takakiyo Nakazawa
Atmos. Meas. Tech., 13, 6703–6731, https://doi.org/10.5194/amt-13-6703-2020, https://doi.org/10.5194/amt-13-6703-2020, 2020
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Air in polar ice cores provides information on past atmosphere and climate. We present a new method for simultaneously measuring eight gases (CH4, N2O and CO2 concentrations; isotopic ratios of N2 and O2; elemental ratios between N2, O2 and Ar; and total air content) from single ice-core samples with high precision.
Bernhard Bereiter, Béla Tuzson, Philipp Scheidegger, André Kupferschmid, Herbert Looser, Lars Mächler, Daniel Baggenstos, Jochen Schmitt, Hubertus Fischer, and Lukas Emmenegger
Atmos. Meas. Tech., 13, 6391–6406, https://doi.org/10.5194/amt-13-6391-2020, https://doi.org/10.5194/amt-13-6391-2020, 2020
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The record of past greenhouse gas composition from ice cores is crucial for our understanding of global climate change. Deciphering this archive requires highly accurate and spatially resolved analysis of the very small amount of gas that is trapped in the ice. This is achieved with a mid-IR laser absorption spectrometer that provides simultaneous, high-precision measurements of CH4, N2O, CO2, and δ13C(CO2) and which will be coupled to a quantitative sublimation extraction method.
Natalie I. Keehan, Bellamy Brownwood, Andrey Marsavin, Douglas A. Day, and Juliane L. Fry
Atmos. Meas. Tech., 13, 6255–6269, https://doi.org/10.5194/amt-13-6255-2020, https://doi.org/10.5194/amt-13-6255-2020, 2020
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This paper describes a new instrument (a thermal-dissociation–cavity ring-down spectrometer, TD-CRDS) for the measurement of key atmospheric gaseous and particle-phase molecules containing the nitrate functional group. Several operational considerations affecting the measurements are described, as well as several characterization experiments comparing the TD-CRDS measurements to analogous measurements from other instruments. Examples are given using a TD-CRDS for ambient and laboratory studies.
Mohammed S. Alam, Leigh R. Crilley, James D. Lee, Louisa J. Kramer, Christian Pfrang, Mónica Vázquez-Moreno, Milagros Ródenas, Amalia Muñoz, and William J. Bloss
Atmos. Meas. Tech., 13, 5977–5991, https://doi.org/10.5194/amt-13-5977-2020, https://doi.org/10.5194/amt-13-5977-2020, 2020
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We report on the interference arising in measurements of nitrogen oxides (NOx) from the presence of a range of alkenes in sampled air when using the most widespread air quality monitoring technique for chemiluminescence detection. Interferences of up to 11 % are reported, depending upon the alkene present and conditions used. Such interferences may be of substantial importance for the interpretation of ambient NOx data, particularly for high volatile organic compound and low NOx environments.
Daniel Marno, Cheryl Ernest, Korbinian Hens, Umar Javed, Thomas Klimach, Monica Martinez, Markus Rudolf, Jos Lelieveld, and Hartwig Harder
Atmos. Meas. Tech., 13, 2711–2731, https://doi.org/10.5194/amt-13-2711-2020, https://doi.org/10.5194/amt-13-2711-2020, 2020
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In this study, a calibration device for OH and HO2 instruments is characterized at pressures of 275 to 1000 mbar, allowing instrument pressure sensitivity to be quantified to an accuracy of 22 % (1σ). Computational fluid dynamic simulations supporting the understanding of interactions between generated HOx and the instrument inlet led to enhanced determination of factors affecting instrument sensitivity.
Joschka Pfeifer, Mario Simon, Martin Heinritzi, Felix Piel, Lena Weitz, Dongyu Wang, Manuel Granzin, Tatjana Müller, Steffen Bräkling, Jasper Kirkby, Joachim Curtius, and Andreas Kürten
Atmos. Meas. Tech., 13, 2501–2522, https://doi.org/10.5194/amt-13-2501-2020, https://doi.org/10.5194/amt-13-2501-2020, 2020
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Ammonia is an important atmospheric trace gas that affects secondary aerosol formation and, together with sulfuric acid, the formation of new particles. A measurement technique is presented that uses high-resolution mass spectrometry and protonated water clusters for the ultrasensitive detection of ammonia at single-digit parts per trillion by volume levels. The instrument is further capable of measuring amines and a suite of iodine compounds at sub-parts per trillion by volume levels.
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Short summary
We have set up a measurement system for methane-clumped isotopologues. We have built an extraction and purification system to extract pure methane for these measurements, for samples of various origins, including atmospheric air, for which we need to process about 1000 L of air for one measurement. We report here the technical setup for extraction and measurements, as well as the calibration, and we give an overview of the samples measured so far.
We have set up a measurement system for methane-clumped isotopologues. We have built an...
