Articles | Volume 21, issue 16
https://doi.org/10.5194/acp-21-12443-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-21-12443-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
19 Aug 2021
Research article |
| 19 Aug 2021
| 19 Aug 2021
Shipborne measurements of methane and carbon dioxide in the Middle East and Mediterranean areas and the contribution from oil and gas emissions
Jean-Daniel Paris
CORRESPONDING AUTHOR
Laboratoire des Sciences du Climat et de l'Environnement,
CEA-CNRS-UVSQ, UMR8212, IPSL, Gif-sur-Yvette, France
Climate and Atmosphere Research Centre (CARE-C), The Cyprus Institute, Nicosia, 2121, Cyprus
Aurélie Riandet
Laboratoire des Sciences du Climat et de l'Environnement,
CEA-CNRS-UVSQ, UMR8212, IPSL, Gif-sur-Yvette, France
now at: Aix Marseille Université, CNRS, Avignon Université, IRD, IMBE, Aix-en-Provence, France
Efstratios Bourtsoukidis
Department of Atmospheric Chemistry, Max Planck Institute for
Chemistry, Mainz 55128, Germany
Climate and Atmosphere Research Centre (CARE-C), The Cyprus Institute, Nicosia, 2121, Cyprus
Marc Delmotte
Laboratoire des Sciences du Climat et de l'Environnement,
CEA-CNRS-UVSQ, UMR8212, IPSL, Gif-sur-Yvette, France
Antoine Berchet
Laboratoire des Sciences du Climat et de l'Environnement,
CEA-CNRS-UVSQ, UMR8212, IPSL, Gif-sur-Yvette, France
Jonathan Williams
Department of Atmospheric Chemistry, Max Planck Institute for
Chemistry, Mainz 55128, Germany
Climate and Atmosphere Research Centre (CARE-C), The Cyprus Institute, Nicosia, 2121, Cyprus
Lisa Ernle
Department of Atmospheric Chemistry, Max Planck Institute for
Chemistry, Mainz 55128, Germany
Ivan Tadic
Department of Atmospheric Chemistry, Max Planck Institute for
Chemistry, Mainz 55128, Germany
Hartwig Harder
Department of Atmospheric Chemistry, Max Planck Institute for
Chemistry, Mainz 55128, Germany
Jos Lelieveld
Department of Atmospheric Chemistry, Max Planck Institute for
Chemistry, Mainz 55128, Germany
Climate and Atmosphere Research Centre (CARE-C), The Cyprus Institute, Nicosia, 2121, Cyprus
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We evaluated how replacing forests with farmland and grazing areas affects atmospheric composition. Using a global climate-chemistry model, we found that deforestation reduces BVOCs, increases farming pollutants, and shifts ozone chemistry. These changes lead to a small cooling effect on the climate. Restoring natural vegetation could reverse some of these effects.
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.
Linda Ort, Andrea Pozzer, Peter Hoor, Florian Obersteiner, Andreas Zahn, Thomas B. Ryerson, Chelsea R. Thompson, Jeff Peischl, Róisín Commane, Bruce Daube, Ilann Bourgeois, Jos Lelieveld, and Horst Fischer
EGUsphere, https://doi.org/10.5194/egusphere-2025-1477, https://doi.org/10.5194/egusphere-2025-1477, 2025
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Pantelis Georgiades, Theo Economou, Yiannis Proestos, Jose Araya, Jos Lelieveld, and Marco Neira
Earth Syst. Sci. Data, 17, 1153–1171, https://doi.org/10.5194/essd-17-1153-2025, https://doi.org/10.5194/essd-17-1153-2025, 2025
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Climate change is posing increasing challenges in the dairy cattle farming sector, as heat stress adversely affects the animals' health and milk production. To accurately assess these impacts, we developed a machine learning model to downscale daily climate data to hourly Temperature Humidity Index (THI) values. We utilized historical weather data to train our model and applied them to future climate projections, under two climate scenarios.
Joël Thanwerdas, Antoine Berchet, Lionel Constantin, Aki Tsuruta, Michael Steiner, Friedemann Reum, Stephan Henne, and Dominik Brunner
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The Community Inversion Framework (CIF) brings together methods for estimating greenhouse gas fluxes from atmospheric observations. The initial ensemble method implemented in CIF was found to be incomplete and could hardly be compared to other ensemble methods employed in the inversion community. In this paper, we present and evaluate a new implementation of the ensemble mode, building upon the initial developments.
Xurong Wang, Alexandra P. Tsimpidi, Zhenqi Luo, Benedikt Steil, Andrea Pozzer, Jos Lelieveld, and Vlassis A. Karydis
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Ammonia (NH3) is an abundant alkaline gas and key precursor in particulate matter formation. While SO2 and NOx emissions have decreased, global NH3 emissions are stable or rising. This study investigates NH3 emission impacts on size-resolved aerosol composition and acidity using the EMAC model, analyzing three emission schemes. Sulphate-nitrate-ammonium aerosols in fine mode sizes are most sensitive to NH3 changes. Regional responses vary. NH3 buffers aerosol acidity, mitigating pH shifts.
Shihan Sun, Paul I. Palmer, Richard Siddans, Brian J. Kerridge, Lucy Ventress, Achim Edtbauer, Akima Ringsdorf, Eva Y. Pfannerstill, and Jonathan Williams
EGUsphere, https://doi.org/10.5194/egusphere-2025-778, https://doi.org/10.5194/egusphere-2025-778, 2025
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Isoprene released by plants can impact atmospheric chemistry and climate. The Amazon rainforest is a major source of isoprene. We derived isoprene emissions using satellite retrievals of isoprene columns and a chemical transport model. We evaluated our isoprene emission estimates using ground-based isoprene observations and satellite retrievals of formaldehyde. We found that using satellite retrievals of isoprene can help better understand isoprene emissions over the Amazon.
Juliette Bernard, Elodie Salmon, Marielle Saunois, Shushi Peng, Penélope Serrano-Ortiz, Antoine Berchet, Palingamoorthy Gnanamoorthy, Joachim Jansen, and Philippe Ciais
Geosci. Model Dev., 18, 863–883, https://doi.org/10.5194/gmd-18-863-2025, https://doi.org/10.5194/gmd-18-863-2025, 2025
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Despite their importance, uncertainties remain in the evaluation of the drivers of temporal variability of methane emissions from wetlands on a global scale. Here, a simplified global model is developed, taking advantage of advances in remote-sensing data and in situ observations. The model reproduces the large spatial and temporal patterns of emissions, albeit with limitations in the tropics due to data scarcity. This model, while simple, can provide valuable insights into sensitivity analyses.
Denis Leppla, Stefanie Hildmann, Nora Zannoni, Leslie Kremper, Bruna Hollanda, Jonathan Williams, Christopher Pöhlker, Stefan Wolff, Marta Sà, Maria Cristina Solci, Ulrich Pöschl, and Thorsten Hoffmann
EGUsphere, https://doi.org/10.5194/egusphere-2025-141, https://doi.org/10.5194/egusphere-2025-141, 2025
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The chemical composition of organic particles in the Amazon rainforest was investigated to understand how biogenic and human emissions influence the atmosphere in this unique ecosystem. Seasonal patterns were found where wet seasons were dominated by biogenic compounds from natural sources while dry seasons showed increased fire-related pollutants. These findings reveal how emissions, fires and long-range transport affect atmospheric chemistry, with implications for climate models.
Ryan Vella, Matthew Forrest, Andrea Pozzer, Alexandra P. Tsimpidi, Thomas Hickler, Jos Lelieveld, and Holger Tost
Atmos. Chem. Phys., 25, 243–262, https://doi.org/10.5194/acp-25-243-2025, https://doi.org/10.5194/acp-25-243-2025, 2025
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This study examines how land cover changes influence biogenic volatile organic compound (BVOC) emissions and atmospheric states. Using a coupled chemistry–climate–vegetation model, we compare present-day land cover (deforested for crops and grazing) with natural vegetation and an extreme reforestation scenario. We find that vegetation changes significantly impact global BVOC emissions and organic aerosols but have a relatively small effect on total aerosols, clouds, and radiative effects.
Akima Ringsdorf, Achim Edtbauer, Bruna Holanda, Christopher Poehlker, Marta O. Sá, Alessandro Araújo, Jürgen Kesselmeier, Jos Lelieveld, and Jonathan Williams
Atmos. Chem. Phys., 24, 11883–11910, https://doi.org/10.5194/acp-24-11883-2024, https://doi.org/10.5194/acp-24-11883-2024, 2024
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We show the average height distribution of separately observed aldehydes and ketones over a day and discuss their rainforest-specific sources and sinks as well as their seasonal changes above the Amazon. Ketones have much longer atmospheric lifetimes than aldehydes and thus different implications for atmospheric chemistry. However, they are commonly observed together, which we overcome by measuring with a NO+ chemical ionization mass spectrometer for the first time in the Amazon rainforest.
Simone T. Andersen, Max R. McGillen, Chaoyang Xue, Tobias Seubert, Patrick Dewald, Gunther N. T. E. Türk, Jan Schuladen, Cyrielle Denjean, Jean-Claude Etienne, Olivier Garrouste, Marina Jamar, Sergio Harb, Manuela Cirtog, Vincent Michoud, Mathieu Cazaunau, Antonin Bergé, Christopher Cantrell, Sebastien Dusanter, Bénédicte Picquet-Varrault, Alexandre Kukui, Abdelwahid Mellouki, Lucy J. Carpenter, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 24, 11603–11618, https://doi.org/10.5194/acp-24-11603-2024, https://doi.org/10.5194/acp-24-11603-2024, 2024
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Using measurements of various trace gases in a suburban forest near Paris in the summer of 2022, we were able to gain insight into the sources and sinks of NOx (NO+NO2) with a special focus on their nighttime chemical and physical loss processes. NO was observed as a result of nighttime soil emissions when O3 levels were strongly depleted by deposition. NO oxidation products were not observed at night, indicating that soil and/or foliar surfaces are an efficient sink of reactive N.
Ana Maria Roxana Petrescu, Glen P. Peters, Richard Engelen, Sander Houweling, Dominik Brunner, Aki Tsuruta, Bradley Matthews, Prabir K. Patra, Dmitry Belikov, Rona L. Thompson, Lena Höglund-Isaksson, Wenxin Zhang, Arjo J. Segers, Giuseppe Etiope, Giancarlo Ciotoli, Philippe Peylin, Frédéric Chevallier, Tuula Aalto, Robbie M. Andrew, David Bastviken, Antoine Berchet, Grégoire Broquet, Giulia Conchedda, Stijn N. C. Dellaert, Hugo Denier van der Gon, Johannes Gütschow, Jean-Matthieu Haussaire, Ronny Lauerwald, Tiina Markkanen, Jacob C. A. van Peet, Isabelle Pison, Pierre Regnier, Espen Solum, Marko Scholze, Maria Tenkanen, Francesco N. Tubiello, Guido R. van der Werf, and John R. Worden
Earth Syst. Sci. Data, 16, 4325–4350, https://doi.org/10.5194/essd-16-4325-2024, https://doi.org/10.5194/essd-16-4325-2024, 2024
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This study provides an overview of data availability from observation- and inventory-based CH4 emission estimates. It systematically compares them and provides recommendations for robust comparisons, aiming to steadily engage more parties in using observational methods to complement their UNFCCC submissions. Anticipating improvements in atmospheric modelling and observations, future developments need to resolve knowledge gaps in both approaches and to better quantify remaining uncertainty.
Josselin Doc, Michel Ramonet, François-Marie Bréon, Delphine Combaz, Mali Chariot, Morgan Lopez, Marc Delmotte, Cristelle Cailteau-Fischbach, Guillaume Nief, Nathanaël Laporte, Thomas Lauvaux, and Philippe Ciais
EGUsphere, https://doi.org/10.5194/egusphere-2024-2826, https://doi.org/10.5194/egusphere-2024-2826, 2024
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Description of the network for measuring greenhouse gas concentrations in the Paris region and analysis of eight years of continuous monitoring.
Pierre Tulet, Joel Van Baelen, Pierre Bosser, Jérome Brioude, Aurélie Colomb, Philippe Goloub, Andrea Pazmino, Thierry Portafaix, Michel Ramonet, Karine Sellegri, Melilotus Thyssen, Léa Gest, Nicolas Marquestaut, Dominique Mékiès, Jean-Marc Metzger, Gilles Athier, Luc Blarel, Marc Delmotte, Guillaume Desprairies, Mérédith Dournaux, Gaël Dubois, Valentin Duflot, Kevin Lamy, Lionel Gardes, Jean-François Guillemot, Valérie Gros, Joanna Kolasinski, Morgan Lopez, Olivier Magand, Erwan Noury, Manuel Nunes-Pinharanda, Guillaume Payen, Joris Pianezze, David Picard, Olivier Picard, Sandrine Prunier, François Rigaud-Louise, Michael Sicard, and Benjamin Torres
Earth Syst. Sci. Data, 16, 3821–3849, https://doi.org/10.5194/essd-16-3821-2024, https://doi.org/10.5194/essd-16-3821-2024, 2024
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The MAP-IO program aims to compensate for the lack of atmospheric and oceanographic observations in the Southern Ocean by equipping the ship Marion Dufresne with a set of 17 scientific instruments. This program collected 700 d of measurements under different latitudes, seasons, sea states, and weather conditions. These new data will support the calibration and validation of numerical models and the understanding of the atmospheric composition of this region of Earth.
Patrick Dewald, Tobias Seubert, Simone T. Andersen, Gunther N. T. E. Türk, Jan Schuladen, Max R. McGillen, Cyrielle Denjean, Jean-Claude Etienne, Olivier Garrouste, Marina Jamar, Sergio Harb, Manuela Cirtog, Vincent Michoud, Mathieu Cazaunau, Antonin Bergé, Christopher Cantrell, Sebastien Dusanter, Bénédicte Picquet-Varrault, Alexandre Kukui, Chaoyang Xue, Abdelwahid Mellouki, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 24, 8983–8997, https://doi.org/10.5194/acp-24-8983-2024, https://doi.org/10.5194/acp-24-8983-2024, 2024
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In the scope of a field campaign in a suburban forest near Paris in the summer of 2022, we measured the reactivity of the nitrate radical NO3 towards biogenic volatile organic compounds (BVOCs; e.g. monoterpenes) mainly below but also above the canopy. NO3 reactivity was the highest during nights with strong temperature inversions and decreased strongly with height. Reactions with BVOCs were the main removal process of NO3 throughout the diel cycle below the canopy.
Luiz A. T. Machado, Jürgen Kesselmeier, Santiago Botía, Hella van Asperen, Meinrat O. Andreae, Alessandro C. de Araújo, Paulo Artaxo, Achim Edtbauer, Rosaria R. Ferreira, Marco A. Franco, Hartwig Harder, Sam P. Jones, Cléo Q. Dias-Júnior, Guido G. Haytzmann, Carlos A. Quesada, Shujiro Komiya, Jost Lavric, Jos Lelieveld, Ingeborg Levin, Anke Nölscher, Eva Pfannerstill, Mira L. Pöhlker, Ulrich Pöschl, Akima Ringsdorf, Luciana Rizzo, Ana M. Yáñez-Serrano, Susan Trumbore, Wanda I. D. Valenti, Jordi Vila-Guerau de Arellano, David Walter, Jonathan Williams, Stefan Wolff, and Christopher Pöhlker
Atmos. Chem. Phys., 24, 8893–8910, https://doi.org/10.5194/acp-24-8893-2024, https://doi.org/10.5194/acp-24-8893-2024, 2024
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Composite analysis of gas concentration before and after rainfall, during the day and night, gives insight into the complex relationship between trace gas variability and precipitation. The analysis helps us to understand the sources and sinks of trace gases within a forest ecosystem. It elucidates processes that are not discernible under undisturbed conditions and contributes to a deeper understanding of the trace gas life cycle and its intricate interactions with cloud dynamics in the Amazon.
Pantelis Georgiades, Matthias Kohl, Mihalis A. Nicolaou, Theodoros Christoudias, Andrea Pozzer, Constantine Dovrolis, and Jos Lelieveld
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2024-314, https://doi.org/10.5194/essd-2024-314, 2024
Manuscript not accepted for further review
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This study maps global ultrafine particle (UFP) concentrations, pollutants known to affect health, using machine learning. By combining environmental and urban data, we predicted UFP levels at a fine 1 km resolution, highlighting areas of high exposure. Our results provide data for public health policies aimed at reducing air pollution impacts. This research bridges data gaps, offering a valuable tool for understanding and mitigating the health effects of UFP exposure.
Anna Martin, Veronika Gayler, Benedikt Steil, Klaus Klingmüller, Patrick Jöckel, Holger Tost, Jos Lelieveld, and Andrea Pozzer
Geosci. Model Dev., 17, 5705–5732, https://doi.org/10.5194/gmd-17-5705-2024, https://doi.org/10.5194/gmd-17-5705-2024, 2024
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The study evaluates the land surface and vegetation model JSBACHv4 as a replacement for the simplified submodel SURFACE in EMAC. JSBACH mitigates earlier problems of soil dryness, which are critical for vegetation modelling. When analysed using different datasets, the coupled model shows strong correlations of key variables, such as land surface temperature, surface albedo and radiation flux. The versatility of the model increases significantly, while the overall performance does not degrade.
Robin Plauchu, Audrey Fortems-Cheiney, Grégoire Broquet, Isabelle Pison, Antoine Berchet, Elise Potier, Gaëlle Dufour, Adriana Coman, Dilek Savas, Guillaume Siour, and Henk Eskes
Atmos. Chem. Phys., 24, 8139–8163, https://doi.org/10.5194/acp-24-8139-2024, https://doi.org/10.5194/acp-24-8139-2024, 2024
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This study uses the Community Inversion Framework and CHIMERE model to assess the potential of TROPOMI-S5P PAL NO2 tropospheric column data to estimate NOx emissions in France (2019–2021). Results show a 3 % decrease in average emissions compared to the 2016 CAMS-REG/INS, lower than the 14 % decrease from CITEPA. The study highlights challenges in capturing emission anomalies due to limited data coverage and error levels but shows promise for local inventory improvements.
Georgia Lazoglou, Theo Economou, Christina Anagnostopoulou, George Zittis, Anna Tzyrkalli, Pantelis Georgiades, and Jos Lelieveld
Geosci. Model Dev., 17, 4689–4703, https://doi.org/10.5194/gmd-17-4689-2024, https://doi.org/10.5194/gmd-17-4689-2024, 2024
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This study focuses on the important issue of the drizzle bias effect in regional climate models, described by an over-prediction of the number of rainy days while underestimating associated precipitation amounts. For this purpose, two distinct methodologies are applied and rigorously evaluated. These results are encouraging for using the multivariate machine learning method random forest to increase the accuracy of climate models concerning the projection of the number of wet days.
Linda Ort, Lenard Lukas Röder, Uwe Parchatka, Rainer Königstedt, Daniel Crowley, Frank Kunz, Ralf Wittkowski, Jos Lelieveld, and Horst Fischer
Atmos. Meas. Tech., 17, 3553–3565, https://doi.org/10.5194/amt-17-3553-2024, https://doi.org/10.5194/amt-17-3553-2024, 2024
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Airborne in situ measurements are of great importance to collect valuable data to improve our knowledge of the atmosphere but also present challenges which demand specific designs. This study presents an IR spectrometer for airborne trace-gas measurements with high data efficiency and a simple, compact design. Its in-flight performance is characterized with the help of a test flight and a comparison with another spectrometer. Moreover, results from its first campaign highlight its benefits.
Sophie Wittig, Antoine Berchet, Isabelle Pison, Marielle Saunois, and Jean-Daniel Paris
Atmos. Chem. Phys., 24, 6359–6373, https://doi.org/10.5194/acp-24-6359-2024, https://doi.org/10.5194/acp-24-6359-2024, 2024
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The aim of this work is to analyse how accurately a methane bomb event could be detected with the current and a hypothetically extended stationary observation network in the Arctic. For this, we incorporate synthetically modelled possible future CH4 concentrations based on plausible emission scenarios into an inverse modelling framework. We analyse how well the increase is detected in different Arctic regions and evaluate the impact of additional observation sites in this respect.
Audrey Fortems-Cheiney, Gregoire Broquet, Elise Potier, Robin Plauchu, Antoine Berchet, Isabelle Pison, Hugo Denier van der Gon, and Stijn Dellaert
Atmos. Chem. Phys., 24, 4635–4649, https://doi.org/10.5194/acp-24-4635-2024, https://doi.org/10.5194/acp-24-4635-2024, 2024
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We have estimated the carbon monixide (CO) European emissions from satellite observations of the MOPITT instrument at the relatively high resolution of 0.5° for a period of over 10 years from 2011 to 2021. The analysis of the inversion results reveals the challenges associated with the inversion of CO emissions at the regional scale over Europe.
Yunsong Liu, Jean-Daniel Paris, Gregoire Broquet, Violeta Bescós Roy, Tania Meixus Fernandez, Rasmus Andersen, Andrés Russu Berlanga, Emil Christensen, Yann Courtois, Sebastian Dominok, Corentin Dussenne, Travis Eckert, Andrew Finlayson, Aurora Fernández de la Fuente, Catlin Gunn, Ram Hashmonay, Juliano Grigoleto Hayashi, Jonathan Helmore, Soeren Honsel, Fabrizio Innocenti, Matti Irjala, Torgrim Log, Cristina Lopez, Francisco Cortés Martínez, Jonathan Martinez, Adrien Massardier, Helle Gottschalk Nygaard, Paula Agregan Reboredo, Elodie Rousset, Axel Scherello, Matthias Ulbricht, Damien Weidmann, Oliver Williams, Nigel Yarrow, Murès Zarea, Robert Ziegler, Jean Sciare, Mihalis Vrekoussis, and Philippe Bousquet
Atmos. Meas. Tech., 17, 1633–1649, https://doi.org/10.5194/amt-17-1633-2024, https://doi.org/10.5194/amt-17-1633-2024, 2024
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We investigated the performance of 10 methane emission quantification techniques in a blind controlled-release experiment at an inerted natural gas compressor station. We reported their respective strengths, weaknesses, and potential complementarity depending on the emission rates and atmospheric conditions. Additionally, we assess the dependence of emission quantification performance on key parameters such as wind speed, deployment constraints, and measurement duration.
Pramod Kumar, Christopher Caldow, Grégoire Broquet, Adil Shah, Olivier Laurent, Camille Yver-Kwok, Sebastien Ars, Sara Defratyka, Susan Warao Gichuki, Luc Lienhardt, Mathis Lozano, Jean-Daniel Paris, Felix Vogel, Caroline Bouchet, Elisa Allegrini, Robert Kelly, Catherine Juery, and Philippe Ciais
Atmos. Meas. Tech., 17, 1229–1250, https://doi.org/10.5194/amt-17-1229-2024, https://doi.org/10.5194/amt-17-1229-2024, 2024
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This study presents a series of mobile measurement campaigns to monitor the CH4 emissions from an active landfill. These measurements are processed using a Gaussian plume model and atmospheric inversion techniques to quantify the landfill CH4 emissions. The methane emission estimates range between ~0.4 and ~7 t CH4 per day, and their variations are analyzed. The robustness of the estimates is assessed depending on the distance of the measurements from the potential sources in the landfill.
Joël Thanwerdas, Marielle Saunois, Antoine Berchet, Isabelle Pison, and Philippe Bousquet
Atmos. Chem. Phys., 24, 2129–2167, https://doi.org/10.5194/acp-24-2129-2024, https://doi.org/10.5194/acp-24-2129-2024, 2024
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We investigate the causes of the renewed growth of atmospheric methane (CH4) after 2007 using inverse modeling. We use the additional information provided by observations of CH4 isotopic compositions to better differentiate between the emission categories. Accounting for the large uncertainties in source signatures, our results suggest that the post-2007 increase in atmospheric CH4 was caused by similar increases in emissions from (1) fossil fuels and (2) agriculture and waste.
Imran A. Girach, Narendra Ojha, Prabha R. Nair, Kandula V. Subrahmanyam, Neelakantan Koushik, Mohammed M. Nazeer, Nadimpally Kiran Kumar, Surendran Nair Suresh Babu, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 24, 1979–1995, https://doi.org/10.5194/acp-24-1979-2024, https://doi.org/10.5194/acp-24-1979-2024, 2024
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We investigate surface ozone variability in East Antarctica based on measurements and EMAC global model simulations during austral summer. Nearly half of the surface ozone is found to be of stratospheric origin. The east coast of Antarctica acts as a stronger sink of ozone than surrounding regions. Photochemical loss of ozone is counterbalanced by downward transport of ozone. The study highlights the intertwined role of chemistry and dynamics in governing ozone variations over East Antarctica.
Ryan Vella, Andrea Pozzer, Matthew Forrest, Jos Lelieveld, Thomas Hickler, and Holger Tost
Biogeosciences, 20, 4391–4412, https://doi.org/10.5194/bg-20-4391-2023, https://doi.org/10.5194/bg-20-4391-2023, 2023
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We investigated the effect of the El Niño–Southern Oscillation (ENSO) on biogenic volatile organic compound (BVOC) emissions from plants. ENSO events can cause a significant increase in these emissions, which have a long-term impact on the Earth's atmosphere. Persistent ENSO conditions can cause long-term changes in vegetation, resulting in even higher BVOC emissions. We link ENSO-induced emission anomalies with driving atmospheric and vegetational variables.
Susanna Strada, Andrea Pozzer, Graziano Giuliani, Erika Coppola, Fabien Solmon, Xiaoyan Jiang, Alex Guenther, Efstratios Bourtsoukidis, Dominique Serça, Jonathan Williams, and Filippo Giorgi
Atmos. Chem. Phys., 23, 13301–13327, https://doi.org/10.5194/acp-23-13301-2023, https://doi.org/10.5194/acp-23-13301-2023, 2023
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Water deficit modifies emissions of isoprene, an aromatic compound released by plants that influences the production of an air pollutant such as ozone. Numerical modelling shows that, during the warmest and driest summers, isoprene decreases between −20 and −60 % over the Euro-Mediterranean region, while near-surface ozone only diminishes by a few percent. Decreases in isoprene emissions not only happen under dry conditions, but also could occur after prolonged or repeated water deficits.
Zaneta Hamryszczak, Antonia Hartmann, Dirk Dienhart, Sascha Hafermann, Bettina Brendel, Rainer Königstedt, Uwe Parchatka, Jos Lelieveld, and Horst Fischer
Atmos. Meas. Tech., 16, 4741–4756, https://doi.org/10.5194/amt-16-4741-2023, https://doi.org/10.5194/amt-16-4741-2023, 2023
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Hydroperoxide measurements improve the understanding of atmospheric oxidation processes. We introduce an instrumental setup for airborne measurements. The aim of the work is the characterization of the measurement method with emphasis on interferences impacting instrumental uncertainty. Technical and physical challenges do not critically impact the instrumental performance. The instrument resolves dynamic processes, such as convective transport, as shown based on the CAFE-Brazil campaign.
Matthias Kohl, Jos Lelieveld, Sourangsu Chowdhury, Sebastian Ehrhart, Disha Sharma, Yafang Cheng, Sachchida Nand Tripathi, Mathew Sebastian, Govindan Pandithurai, Hongli Wang, and Andrea Pozzer
Atmos. Chem. Phys., 23, 13191–13215, https://doi.org/10.5194/acp-23-13191-2023, https://doi.org/10.5194/acp-23-13191-2023, 2023
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Knowledge on atmospheric ultrafine particles (UFPs) with a diameter smaller than 100 nm is crucial for public health and the hydrological cycle. We present a new global dataset of UFP concentrations at the Earth's surface derived with a comprehensive chemistry–climate model and evaluated with ground-based observations. The evaluation results are combined with high-resolution primary emissions to downscale UFP concentrations to an unprecedented horizontal resolution of 0.1° × 0.1°.
Clara M. Nussbaumer, Horst Fischer, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 23, 12651–12669, https://doi.org/10.5194/acp-23-12651-2023, https://doi.org/10.5194/acp-23-12651-2023, 2023
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Ozone is a greenhouse gas and contributes to the earth’s radiative energy budget and therefore to global warming. This effect is the largest in the upper troposphere. In this study, we investigate the processes controlling ozone formation and the sensitivity to its precursors in the upper tropical troposphere based on model simulations by the ECHAM5/MESSy2 Atmospheric Chemistry (EMAC) model. We find that NO𝑥 emissions from lightning most importantly affect ozone chemistry at these altitudes.
Matthew J. McGrath, Ana Maria Roxana Petrescu, Philippe Peylin, Robbie M. Andrew, Bradley Matthews, Frank Dentener, Juraj Balkovič, Vladislav Bastrikov, Meike Becker, Gregoire Broquet, Philippe Ciais, Audrey Fortems-Cheiney, Raphael Ganzenmüller, Giacomo Grassi, Ian Harris, Matthew Jones, Jürgen Knauer, Matthias Kuhnert, Guillaume Monteil, Saqr Munassar, Paul I. Palmer, Glen P. Peters, Chunjing Qiu, Mart-Jan Schelhaas, Oksana Tarasova, Matteo Vizzarri, Karina Winkler, Gianpaolo Balsamo, Antoine Berchet, Peter Briggs, Patrick Brockmann, Frédéric Chevallier, Giulia Conchedda, Monica Crippa, Stijn N. C. Dellaert, Hugo A. C. Denier van der Gon, Sara Filipek, Pierre Friedlingstein, Richard Fuchs, Michael Gauss, Christoph Gerbig, Diego Guizzardi, Dirk Günther, Richard A. Houghton, Greet Janssens-Maenhout, Ronny Lauerwald, Bas Lerink, Ingrid T. Luijkx, Géraud Moulas, Marilena Muntean, Gert-Jan Nabuurs, Aurélie Paquirissamy, Lucia Perugini, Wouter Peters, Roberto Pilli, Julia Pongratz, Pierre Regnier, Marko Scholze, Yusuf Serengil, Pete Smith, Efisio Solazzo, Rona L. Thompson, Francesco N. Tubiello, Timo Vesala, and Sophia Walther
Earth Syst. Sci. Data, 15, 4295–4370, https://doi.org/10.5194/essd-15-4295-2023, https://doi.org/10.5194/essd-15-4295-2023, 2023
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Accurate estimation of fluxes of carbon dioxide from the land surface is essential for understanding future impacts of greenhouse gas emissions on the climate system. A wide variety of methods currently exist to estimate these sources and sinks. We are continuing work to develop annual comparisons of these diverse methods in order to clarify what they all actually calculate and to resolve apparent disagreement, in addition to highlighting opportunities for increased understanding.
Sara M. Defratyka, James L. France, Rebecca E. Fisher, Dave Lowry, Julianne M. Fernandez, Semra Bakkaloglu, Camille Yver-Kwok, Jean-Daniel Paris, Philippe Bousquet, Tim Arnold, Chris Rennick, Jon Helmore, Nigel Yarrow, and Euan G. Nisbet
EGUsphere, https://doi.org/10.5194/egusphere-2023-1490, https://doi.org/10.5194/egusphere-2023-1490, 2023
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We are focused on verification of δ13CH4 measurements in near-source conditions and we have provided an insight into the impact of chosen calculation methods for determined isotopic signatures. Our study offers a step forward for establishing an unified, robust, and reliable analytical technique to determine δ13CH4 of methane sources. Our recommended analytical approach reduces biases and uncertainties coming from measurement conditions, data clustering and various available fitting methods.
Eliane Gomes Alves, Raoni Aquino Santana, Cléo Quaresma Dias-Júnior, Santiago Botía, Tyeen Taylor, Ana Maria Yáñez-Serrano, Jürgen Kesselmeier, Efstratios Bourtsoukidis, Jonathan Williams, Pedro Ivo Lembo Silveira de Assis, Giordane Martins, Rodrigo de Souza, Sérgio Duvoisin Júnior, Alex Guenther, Dasa Gu, Anywhere Tsokankunku, Matthias Sörgel, Bruce Nelson, Davieliton Pinto, Shujiro Komiya, Diogo Martins Rosa, Bettina Weber, Cybelli Barbosa, Michelle Robin, Kenneth J. Feeley, Alvaro Duque, Viviana Londoño Lemos, Maria Paula Contreras, Alvaro Idarraga, Norberto López, Chad Husby, Brett Jestrow, and Iván Mauricio Cely Toro
Atmos. Chem. Phys., 23, 8149–8168, https://doi.org/10.5194/acp-23-8149-2023, https://doi.org/10.5194/acp-23-8149-2023, 2023
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Isoprene is emitted mainly by plants and can influence atmospheric chemistry and air quality. But, there are uncertainties in model emission estimates and follow-up atmospheric processes. In our study, with long-term observational datasets of isoprene and biological and environmental factors from central Amazonia, we show that isoprene emission estimates could be improved when biological processes were mechanistically incorporated into the model.
Seyed Omid Nabavi, Theodoros Christoudias, Yiannis Proestos, Christos Fountoukis, Huda Al-Sulaiti, and Jos Lelieveld
Atmos. Chem. Phys., 23, 7719–7739, https://doi.org/10.5194/acp-23-7719-2023, https://doi.org/10.5194/acp-23-7719-2023, 2023
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The objective of our study is to comprehensively assess the timing of radioactive material transportation and deposition, along with the associated population exposure in the designated region. We employed diverse meteorological inputs, emission specifics, and simulation codes, aiming to quantify the level of uncertainty.
Sophie Wittig, Antoine Berchet, Isabelle Pison, Marielle Saunois, Joël Thanwerdas, Adrien Martinez, Jean-Daniel Paris, Toshinobu Machida, Motoki Sasakawa, Douglas E. J. Worthy, Xin Lan, Rona L. Thompson, Espen Sollum, and Mikhail Arshinov
Atmos. Chem. Phys., 23, 6457–6485, https://doi.org/10.5194/acp-23-6457-2023, https://doi.org/10.5194/acp-23-6457-2023, 2023
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Here, an inverse modelling approach is applied to estimate CH4 sources and sinks in the Arctic from 2008 to 2019. We study the magnitude, seasonal patterns and trends from different sources during recent years. We also assess how the current observation network helps to constrain fluxes. We find that constraints are only significant for North America and, to a lesser extent, West Siberia, where the observation network is relatively dense. We find no clear trend over the period of inversion.
Klaus Klingmüller and Jos Lelieveld
Geosci. Model Dev., 16, 3013–3028, https://doi.org/10.5194/gmd-16-3013-2023, https://doi.org/10.5194/gmd-16-3013-2023, 2023
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Desert dust has significant impacts on climate, public health, infrastructure and ecosystems. An impact assessment requires numerical predictions, which are challenging because the dust emissions are not well known. We present a novel approach using satellite observations and machine learning to more accurately estimate the emissions and to improve the model simulations.
Zaneta Hamryszczak, Dirk Dienhart, Bettina Brendel, Roland Rohloff, Daniel Marno, Monica Martinez, Hartwig Harder, Andrea Pozzer, Birger Bohn, Martin Zöger, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 23, 5929–5943, https://doi.org/10.5194/acp-23-5929-2023, https://doi.org/10.5194/acp-23-5929-2023, 2023
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Hydrogen peroxide is a key contributor to the oxidative chemistry of the atmosphere through its link to the most prominent oxidants controlling its self-cleansing capacity, HOx. During the CAFE-Africa campaign, H2O2 was measured over the Atlantic Ocean and western Africa in August/September 2018. The study gives an overview of the distribution of H2O2 in the upper tropical troposphere and investigates the impact of convective processes in the Intertropical Convergence Zone on the budget of H2O2.
Ana Maria Roxana Petrescu, Chunjing Qiu, Matthew J. McGrath, Philippe Peylin, Glen P. Peters, Philippe Ciais, Rona L. Thompson, Aki Tsuruta, Dominik Brunner, Matthias Kuhnert, Bradley Matthews, Paul I. Palmer, Oksana Tarasova, Pierre Regnier, Ronny Lauerwald, David Bastviken, Lena Höglund-Isaksson, Wilfried Winiwarter, Giuseppe Etiope, Tuula Aalto, Gianpaolo Balsamo, Vladislav Bastrikov, Antoine Berchet, Patrick Brockmann, Giancarlo Ciotoli, Giulia Conchedda, Monica Crippa, Frank Dentener, Christine D. Groot Zwaaftink, Diego Guizzardi, Dirk Günther, Jean-Matthieu Haussaire, Sander Houweling, Greet Janssens-Maenhout, Massaer Kouyate, Adrian Leip, Antti Leppänen, Emanuele Lugato, Manon Maisonnier, Alistair J. Manning, Tiina Markkanen, Joe McNorton, Marilena Muntean, Gabriel D. Oreggioni, Prabir K. Patra, Lucia Perugini, Isabelle Pison, Maarit T. Raivonen, Marielle Saunois, Arjo J. Segers, Pete Smith, Efisio Solazzo, Hanqin Tian, Francesco N. Tubiello, Timo Vesala, Guido R. van der Werf, Chris Wilson, and Sönke Zaehle
Earth Syst. Sci. Data, 15, 1197–1268, https://doi.org/10.5194/essd-15-1197-2023, https://doi.org/10.5194/essd-15-1197-2023, 2023
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This study updates the state-of-the-art scientific overview of CH4 and N2O emissions in the EU27 and UK in Petrescu et al. (2021a). Yearly updates are needed to improve the different respective approaches and to inform on the development of formal verification systems. It integrates the most recent emission inventories, process-based model and regional/global inversions, comparing them with UNFCCC national GHG inventories, in support to policy to facilitate real-time verification procedures.
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.
Lenard L. Röder, Patrick Dewald, Clara M. Nussbaumer, Jan Schuladen, John N. Crowley, Jos Lelieveld, and Horst Fischer
Atmos. Meas. Tech., 16, 1167–1178, https://doi.org/10.5194/amt-16-1167-2023, https://doi.org/10.5194/amt-16-1167-2023, 2023
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Field experiments in atmospheric chemistry provide insights into chemical interactions of our atmosphere. However, high data coverage and accuracy are needed to enable further analysis. In this study, we explore a statistical method that combines knowledge about the chemical reactions with information from measurements to increase the quality of field experiment datasets. We test the algorithm for several applications and discuss limitations that depend on the specific variable and the dynamics.
Clément Narbaud, Jean-Daniel Paris, Sophie Wittig, Antoine Berchet, Marielle Saunois, Philippe Nédélec, Boris D. Belan, Mikhail Y. Arshinov, Sergei B. Belan, Denis Davydov, Alexander Fofonov, and Artem Kozlov
Atmos. Chem. Phys., 23, 2293–2314, https://doi.org/10.5194/acp-23-2293-2023, https://doi.org/10.5194/acp-23-2293-2023, 2023
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We measured CH4 and CO2 from aircraft over the Russian Arctic. Analyzing our data with the Lagrangian model FLEXPART, we find a sharp east–west gradient in atmospheric composition. Western Siberia is influenced by strong wetland CH4 emissions, deep CO2 gradient from biospheric uptake, and long-range transport from Europe and North America. Eastern flights document less variability. Over the Arctic Ocean, we find a small influence from marine CH4 emissions compatible with reasonable inventories.
Ryan Vella, Matthew Forrest, Jos Lelieveld, and Holger Tost
Geosci. Model Dev., 16, 885–906, https://doi.org/10.5194/gmd-16-885-2023, https://doi.org/10.5194/gmd-16-885-2023, 2023
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Biogenic volatile organic compounds (BVOCs) are released by vegetation and have a major impact on atmospheric chemistry and aerosol formation. Non-interacting vegetation constrains the majority of numerical models used to estimate global BVOC emissions, and thus, the effects of changing vegetation on emissions are not addressed. In this work, we replace the offline vegetation with dynamic vegetation states by linking a chemistry–climate model with a global dynamic vegetation model.
Jennifer Schallock, Christoph Brühl, Christine Bingen, Michael Höpfner, Landon Rieger, and Jos Lelieveld
Atmos. Chem. Phys., 23, 1169–1207, https://doi.org/10.5194/acp-23-1169-2023, https://doi.org/10.5194/acp-23-1169-2023, 2023
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We characterized the influence of volcanic aerosols for the period 1990–2019 and established a volcanic SO2 emission inventory that includes more than 500 eruptions. From limb-based satellite observations of SO2 and extinction, we derive 3D plumes of SO2 perturbations and injected mass by a novel method. We calculate instantaneous radiative forcing with a comprehensive chemisty climate model. Our results show that smaller eruptions can also contribute to the stratospheric aerosol forcing.
Denis Leppla, Nora Zannoni, Leslie Kremper, Jonathan Williams, Christopher Pöhlker, Marta Sá, Maria Christina Solci, and Thorsten Hoffmann
Atmos. Chem. Phys., 23, 809–820, https://doi.org/10.5194/acp-23-809-2023, https://doi.org/10.5194/acp-23-809-2023, 2023
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Chiral chemodiversity plays a critical role in biochemical processes such as insect and plant communication. Here we report on the measurement of chiral-specified secondary organic aerosol in the Amazon rainforest. The results show that the chiral ratio is mainly determined by large-scale emission processes. Characteristic emissions of chiral aerosol precursors from different forest ecosystems can thus provide large-scale information on different biogenic sources via chiral particle analysis.
Mohamed Abdelkader, Georgiy Stenchikov, Andrea Pozzer, Holger Tost, and Jos Lelieveld
Atmos. Chem. Phys., 23, 471–500, https://doi.org/10.5194/acp-23-471-2023, https://doi.org/10.5194/acp-23-471-2023, 2023
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We study the effect of injected volcanic ash, water vapor, and SO2 on the development of the volcanic cloud and the stratospheric aerosol optical depth (AOD). Both are sensitive to the initial injection height and to the aging of the volcanic ash shaped by heterogeneous chemistry coupled with the ozone cycle. The paper explains the large differences in AOD for different injection scenarios, which could improve the estimate of the radiative forcing of volcanic eruptions.
Dirk Dienhart, Bettina Brendel, John N. Crowley, Philipp G. Eger, Hartwig Harder, Monica Martinez, Andrea Pozzer, Roland Rohloff, Jan Schuladen, Sebastian Tauer, David Walter, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 23, 119–142, https://doi.org/10.5194/acp-23-119-2023, https://doi.org/10.5194/acp-23-119-2023, 2023
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Formaldehyde and hydroperoxide measurements were performed in the marine boundary layer around the Arabian Peninsula and highlight the Suez Canal and Arabian (Persian) Gulf as a hotspot of photochemical air pollution. A comparison with the EMAC model shows that the formaldehyde results match within a factor of 2, while hydrogen peroxide was overestimated by more than a factor of 5, which revealed enhanced HOx (OH+HO2) radicals in the simulation and an underestimation of dry deposition velocites.
Joël Thanwerdas, Marielle Saunois, Isabelle Pison, Didier Hauglustaine, Antoine Berchet, Bianca Baier, Colm Sweeney, and Philippe Bousquet
Atmos. Chem. Phys., 22, 15489–15508, https://doi.org/10.5194/acp-22-15489-2022, https://doi.org/10.5194/acp-22-15489-2022, 2022
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Atmospheric methane (CH4) concentrations have been rising since 2007, resulting from an imbalance between CH4 sources and sinks. The CH4 budget is generally estimated through top-down approaches using CH4 and δ13C(CH4) observations as constraints. The oxidation by chlorine (Cl) contributes little to the total oxidation of CH4 but strongly influences δ13C(CH4). Here, we compare multiple recent Cl fields and quantify the influence of Cl concentrations on CH4, δ13C(CH4), and CH4 budget estimates.
Laura Tomsche, Andreas Marsing, Tina Jurkat-Witschas, Johannes Lucke, Stefan Kaufmann, Katharina Kaiser, Johannes Schneider, Monika Scheibe, Hans Schlager, Lenard Röder, Horst Fischer, Florian Obersteiner, Andreas Zahn, Martin Zöger, Jos Lelieveld, and Christiane Voigt
Atmos. Chem. Phys., 22, 15135–15151, https://doi.org/10.5194/acp-22-15135-2022, https://doi.org/10.5194/acp-22-15135-2022, 2022
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The detection of sulfur compounds in the upper troposphere (UT) and lower stratosphere (LS) is a challenge. In-flight measurements of SO2 and sulfate aerosol were performed during the BLUESKY mission in spring 2020 under exceptional atmospheric conditions. Reduced sinks in the dry UTLS and lower but still significant air traffic influenced the enhanced SO2 in the UT, and aged volcanic plumes enhanced the LS sulfate aerosol impacting the atmospheric radiation budget and global climate.
Peter Bergamaschi, Arjo Segers, Dominik Brunner, Jean-Matthieu Haussaire, Stephan Henne, Michel Ramonet, Tim Arnold, Tobias Biermann, Huilin Chen, Sebastien Conil, Marc Delmotte, Grant Forster, Arnoud Frumau, Dagmar Kubistin, Xin Lan, Markus Leuenberger, Matthias Lindauer, Morgan Lopez, Giovanni Manca, Jennifer Müller-Williams, Simon O'Doherty, Bert Scheeren, Martin Steinbacher, Pamela Trisolino, Gabriela Vítková, and Camille Yver Kwok
Atmos. Chem. Phys., 22, 13243–13268, https://doi.org/10.5194/acp-22-13243-2022, https://doi.org/10.5194/acp-22-13243-2022, 2022
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We present a novel high-resolution inverse modelling system, "FLEXVAR", and its application for the inverse modelling of European CH4 emissions in 2018. The new system combines a high spatial resolution of 7 km x 7 km with a variational data assimilation technique, which allows CH4 emissions to be optimized from individual model grid cells. The high resolution allows the observations to be better reproduced, while the derived emissions show overall good consistency with two existing models.
Charlotte M. Beall, Thomas C. J. Hill, Paul J. DeMott, Tobias Köneman, Michael Pikridas, Frank Drewnick, Hartwig Harder, Christopher Pöhlker, Jos Lelieveld, Bettina Weber, Minas Iakovides, Roman Prokeš, Jean Sciare, Meinrat O. Andreae, M. Dale Stokes, and Kimberly A. Prather
Atmos. Chem. Phys., 22, 12607–12627, https://doi.org/10.5194/acp-22-12607-2022, https://doi.org/10.5194/acp-22-12607-2022, 2022
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Ice-nucleating particles (INPs) are rare aerosols that can trigger ice formation in clouds and affect climate-relevant cloud properties such as phase, reflectivity and lifetime. Dust is the dominant INP source, yet few measurements have been reported near major dust sources. We report INP observations within hundreds of kilometers of the biggest dust source regions globally: the Sahara and the Arabian Peninsula. Results show that at temperatures > −15 °C, INPs are dominated by organics.
Mengze Li, Andrea Pozzer, Jos Lelieveld, and Jonathan Williams
Earth Syst. Sci. Data, 14, 4351–4364, https://doi.org/10.5194/essd-14-4351-2022, https://doi.org/10.5194/essd-14-4351-2022, 2022
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We present a northern hemispheric airborne measurement dataset of atmospheric ethane, propane and methane and temporal trends for the time period 2006–2016 in the upper troposphere and lower stratosphere. The growth rates of ethane, methane, and propane in the upper troposphere are -2.24, 0.33, and -0.78 % yr-1, respectively, and in the lower stratosphere they are -3.27, 0.26, and -4.91 % yr-1, respectively, in 2006–2016.
Therese S. Carter, Colette L. Heald, Jesse H. Kroll, Eric C. Apel, Donald Blake, Matthew Coggon, Achim Edtbauer, Georgios Gkatzelis, Rebecca S. Hornbrook, Jeff Peischl, Eva Y. Pfannerstill, Felix Piel, Nina G. Reijrink, Akima Ringsdorf, Carsten Warneke, Jonathan Williams, Armin Wisthaler, and Lu Xu
Atmos. Chem. Phys., 22, 12093–12111, https://doi.org/10.5194/acp-22-12093-2022, https://doi.org/10.5194/acp-22-12093-2022, 2022
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Fires emit many gases which can contribute to smog and air pollution. However, the amount and properties of these chemicals are not well understood, so this work updates and expands their representation in a global atmospheric model, including by adding new chemicals. We confirm that this updated representation generally matches measurements taken in several fire regions. We then show that fires provide ~15 % of atmospheric reactivity globally and more than 75 % over fire source regions.
Elise Potier, Grégoire Broquet, Yilong Wang, Diego Santaren, Antoine Berchet, Isabelle Pison, Julia Marshall, Philippe Ciais, François-Marie Bréon, and Frédéric Chevallier
Atmos. Meas. Tech., 15, 5261–5288, https://doi.org/10.5194/amt-15-5261-2022, https://doi.org/10.5194/amt-15-5261-2022, 2022
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Atmospheric inversion at local–regional scales over Europe and pseudo-data assimilation are used to evaluate how CO2 and 14CO2 ground-based measurement networks could complement satellite CO2 imagers to monitor fossil fuel (FF) CO2 emissions. This combination significantly improves precision in the FF emission estimates in areas with a dense network but does not strongly support the separation of the FF from the biogenic signals or the spatio-temporal extrapolation of the satellite information.
Simon F. Reifenberg, Anna Martin, Matthias Kohl, Sara Bacer, Zaneta Hamryszczak, Ivan Tadic, Lenard Röder, Daniel J. Crowley, Horst Fischer, Katharina Kaiser, Johannes Schneider, Raphael Dörich, John N. Crowley, Laura Tomsche, Andreas Marsing, Christiane Voigt, Andreas Zahn, Christopher Pöhlker, Bruna A. Holanda, Ovid Krüger, Ulrich Pöschl, Mira Pöhlker, Patrick Jöckel, Marcel Dorf, Ulrich Schumann, Jonathan Williams, Birger Bohn, Joachim Curtius, Hardwig Harder, Hans Schlager, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 22, 10901–10917, https://doi.org/10.5194/acp-22-10901-2022, https://doi.org/10.5194/acp-22-10901-2022, 2022
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In this work we use a combination of observational data from an aircraft campaign and model results to investigate the effect of the European lockdown due to COVID-19 in spring 2020. Using model results, we show that the largest relative changes to the atmospheric composition caused by the reduced emissions are located in the upper troposphere around aircraft cruise altitude, while the largest absolute changes are present at the surface.
Yunsong Liu, Jean-Daniel Paris, Mihalis Vrekoussis, Panayiota Antoniou, Christos Constantinides, Maximilien Desservettaz, Christos Keleshis, Olivier Laurent, Andreas Leonidou, Carole Philippon, Panagiotis Vouterakos, Pierre-Yves Quéhé, Philippe Bousquet, and Jean Sciare
Atmos. Meas. Tech., 15, 4431–4442, https://doi.org/10.5194/amt-15-4431-2022, https://doi.org/10.5194/amt-15-4431-2022, 2022
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This paper details laboratory-based and field developments of a cost-effective and compacted UAV CO2 sensor system to address the challenge of measuring CO2 with sufficient precision and acquisition frequency. We assess its performance extensively through laboratory and field tests and provide a case study in an urban area (Nicosia, Cyprus). We therefore expect that this portable system will be widely used for measuring CO2 emission and distribution in natural or urban environments.
Zaneta T. Hamryszczak, Andrea Pozzer, Florian Obersteiner, Birger Bohn, Benedikt Steil, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 22, 9483–9497, https://doi.org/10.5194/acp-22-9483-2022, https://doi.org/10.5194/acp-22-9483-2022, 2022
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Hydrogen peroxide plays a pivotal role in the chemistry of the atmosphere. Together with organic hydroperoxides, it forms a reservoir for peroxy radicals, which are known to be the key contributors to the self-cleaning processes of the atmosphere. Hydroperoxides were measured over Europe during the BLUESKY campaign in May–June 2020. The paper gives an overview of the distribution of the species in the troposphere and investigates the impact of wet scavenging and deposition on the budget of H2O2.
Marco Wietzoreck, Marios Kyprianou, Benjamin A. Musa Bandowe, Siddika Celik, John N. Crowley, Frank Drewnick, Philipp Eger, Nils Friedrich, Minas Iakovides, Petr Kukučka, Jan Kuta, Barbora Nežiková, Petra Pokorná, Petra Přibylová, Roman Prokeš, Roland Rohloff, Ivan Tadic, Sebastian Tauer, Jake Wilson, Hartwig Harder, Jos Lelieveld, Ulrich Pöschl, Euripides G. Stephanou, and Gerhard Lammel
Atmos. Chem. Phys., 22, 8739–8766, https://doi.org/10.5194/acp-22-8739-2022, https://doi.org/10.5194/acp-22-8739-2022, 2022
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A unique dataset of concentrations and sources of polycyclic aromatic hydrocarbons (PAHs) and their alkylated, oxygenated and nitrated derivatives, in total 74 individual species, in the marine atmosphere is presented. Exposure to these substances poses a major health risk. We found very low concentrations over the Arabian Sea, while both local and long-range-transported pollution caused elevated levels over the Mediterranean Sea and the Arabian Gulf.
Ovid O. Krüger, Bruna A. Holanda, Sourangsu Chowdhury, Andrea Pozzer, David Walter, Christopher Pöhlker, Maria Dolores Andrés Hernández, John P. Burrows, Christiane Voigt, Jos Lelieveld, Johannes Quaas, Ulrich Pöschl, and Mira L. Pöhlker
Atmos. Chem. Phys., 22, 8683–8699, https://doi.org/10.5194/acp-22-8683-2022, https://doi.org/10.5194/acp-22-8683-2022, 2022
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The abrupt reduction in human activities during the first COVID-19 lockdown created unprecedented atmospheric conditions. We took the opportunity to quantify changes in black carbon (BC) as a major anthropogenic air pollutant. Therefore, we measured BC on board a research aircraft over Europe during the lockdown and compared the results to measurements from 2017. With model simulations we account for different weather conditions and find a lockdown-related decrease in BC of 41 %.
Boris D. Belan, Gerard Ancellet, Irina S. Andreeva, Pavel N. Antokhin, Viktoria G. Arshinova, Mikhail Y. Arshinov, Yurii S. Balin, Vladimir E. Barsuk, Sergei B. Belan, Dmitry G. Chernov, Denis K. Davydov, Alexander V. Fofonov, Georgii A. Ivlev, Sergei N. Kotel'nikov, Alexander S. Kozlov, Artem V. Kozlov, Katharine Law, Andrey V. Mikhal'chishin, Igor A. Moseikin, Sergei V. Nasonov, Philippe Nédélec, Olesya V. Okhlopkova, Sergei E. Ol'kin, Mikhail V. Panchenko, Jean-Daniel Paris, Iogannes E. Penner, Igor V. Ptashnik, Tatyana M. Rasskazchikova, Irina K. Reznikova, Oleg A. Romanovskii, Alexander S. Safatov, Denis E. Savkin, Denis V. Simonenkov, Tatyana K. Sklyadneva, Gennadii N. Tolmachev, Semyon V. Yakovlev, and Polina N. Zenkova
Atmos. Meas. Tech., 15, 3941–3967, https://doi.org/10.5194/amt-15-3941-2022, https://doi.org/10.5194/amt-15-3941-2022, 2022
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The change of the global climate is most pronounced in the Arctic, where the air temperature increases faster than the global average. This is associated with an increase in the concentration of greenhouse gases in the atmosphere. It is important to study how the air composition in the Arctic changes in the changing climate. Thus this integrated experiment was carried out to measure the composition of the troposphere in the Russian sector of the Arctic from on board the aircraft laboratory.
Joël Thanwerdas, Marielle Saunois, Antoine Berchet, Isabelle Pison, Bruce H. Vaughn, Sylvia Englund Michel, and Philippe Bousquet
Geosci. Model Dev., 15, 4831–4851, https://doi.org/10.5194/gmd-15-4831-2022, https://doi.org/10.5194/gmd-15-4831-2022, 2022
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Estimating CH4 sources by exploiting observations within an inverse modeling framework is a powerful approach. Here, a new system designed to assimilate δ13C(CH4) observations together with CH4 observations is presented. By optimizing both the emissions and associated source signatures of multiple emission categories, this new system can efficiently differentiate the co-located emission categories and provide estimates of CH4 sources that are consistent with isotopic data.
Patrick Dewald, Clara M. Nussbaumer, Jan Schuladen, Akima Ringsdorf, Achim Edtbauer, Horst Fischer, Jonathan Williams, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 22, 7051–7069, https://doi.org/10.5194/acp-22-7051-2022, https://doi.org/10.5194/acp-22-7051-2022, 2022
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We measured the gas-phase reactivity of the NO3 radical on the summit (825 m a.s.l.) of a semi-rural mountain in southwestern Germany in July 2021. The impact of VOC-induced NO3 losses (mostly monoterpenes) competing with a loss by reaction with NO and photolysis throughout the diel cycle was estimated. Besides chemistry, boundary layer dynamics and plant-physiological processes presumably have a great impact on our observations, which were compared to previous NO3 measurements at the same site.
George K. Georgiou, Theodoros Christoudias, Yiannis Proestos, Jonilda Kushta, Michael Pikridas, Jean Sciare, Chrysanthos Savvides, and Jos Lelieveld
Geosci. Model Dev., 15, 4129–4146, https://doi.org/10.5194/gmd-15-4129-2022, https://doi.org/10.5194/gmd-15-4129-2022, 2022
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We evaluate the skill of the WRF-Chem model to perform high-resolution air quality forecasts (including ozone, nitrogen dioxide, and fine particulate matter) over the Eastern Mediterranean, during winter and summer. We compare the forecast output to observational data from background and urban locations and the forecast output from CAMS. WRF-Chem was found to forecast the concentrations and diurnal profiles of gas-phase pollutants in urban areas with higher accuracy.
Clara M. Nussbaumer, Andrea Pozzer, Ivan Tadic, Lenard Röder, Florian Obersteiner, Hartwig Harder, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 22, 6151–6165, https://doi.org/10.5194/acp-22-6151-2022, https://doi.org/10.5194/acp-22-6151-2022, 2022
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The European COVID-19 lockdowns have significantly reduced the emission of primary pollutants such as NOx, which impacts the tropospheric photochemical processes and the abundance of O3. In this study, we present how the lockdowns have affected tropospheric trace gases and ozone production based on in situ observations and modeling simulations. We additionally show that the chemical regime shifted from a transition point to a NOx limitation in the upper troposphere.
Wenyu Sun, Matias Berasategui, Andrea Pozzer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 22, 4969–4984, https://doi.org/10.5194/acp-22-4969-2022, https://doi.org/10.5194/acp-22-4969-2022, 2022
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The reaction between OH and SO2 is a termolecular process that in the atmosphere results in the formation of H2SO4 and thus aerosols. We present the first temperature- and pressure-dependent measurements of the rate coefficients in N2. This is also the first study to examine the effects of water vapour on the kinetics of this reaction. Our results indicate the rate coefficient is larger than that recommended by evaluation panels, with deviations of up to 30 % in some parts of the atmosphere.
Hanna K. Lappalainen, Tuukka Petäjä, Timo Vihma, Jouni Räisänen, Alexander Baklanov, Sergey Chalov, Igor Esau, Ekaterina Ezhova, Matti Leppäranta, Dmitry Pozdnyakov, Jukka Pumpanen, Meinrat O. Andreae, Mikhail Arshinov, Eija Asmi, Jianhui Bai, Igor Bashmachnikov, Boris Belan, Federico Bianchi, Boris Biskaborn, Michael Boy, Jaana Bäck, Bin Cheng, Natalia Chubarova, Jonathan Duplissy, Egor Dyukarev, Konstantinos Eleftheriadis, Martin Forsius, Martin Heimann, Sirkku Juhola, Vladimir Konovalov, Igor Konovalov, Pavel Konstantinov, Kajar Köster, Elena Lapshina, Anna Lintunen, Alexander Mahura, Risto Makkonen, Svetlana Malkhazova, Ivan Mammarella, Stefano Mammola, Stephany Buenrostro Mazon, Outi Meinander, Eugene Mikhailov, Victoria Miles, Stanislav Myslenkov, Dmitry Orlov, Jean-Daniel Paris, Roberta Pirazzini, Olga Popovicheva, Jouni Pulliainen, Kimmo Rautiainen, Torsten Sachs, Vladimir Shevchenko, Andrey Skorokhod, Andreas Stohl, Elli Suhonen, Erik S. Thomson, Marina Tsidilina, Veli-Pekka Tynkkynen, Petteri Uotila, Aki Virkkula, Nadezhda Voropay, Tobias Wolf, Sayaka Yasunaka, Jiahua Zhang, Yubao Qiu, Aijun Ding, Huadong Guo, Valery Bondur, Nikolay Kasimov, Sergej Zilitinkevich, Veli-Matti Kerminen, and Markku Kulmala
Atmos. Chem. Phys., 22, 4413–4469, https://doi.org/10.5194/acp-22-4413-2022, https://doi.org/10.5194/acp-22-4413-2022, 2022
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We summarize results during the last 5 years in the northern Eurasian region, especially from Russia, and introduce recent observations of the air quality in the urban environments in China. Although the scientific knowledge in these regions has increased, there are still gaps in our understanding of large-scale climate–Earth surface interactions and feedbacks. This arises from limitations in research infrastructures and integrative data analyses, hindering a comprehensive system analysis.
Marine Remaud, Frédéric Chevallier, Fabienne Maignan, Sauveur Belviso, Antoine Berchet, Alexandra Parouffe, Camille Abadie, Cédric Bacour, Sinikka Lennartz, and Philippe Peylin
Atmos. Chem. Phys., 22, 2525–2552, https://doi.org/10.5194/acp-22-2525-2022, https://doi.org/10.5194/acp-22-2525-2022, 2022
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Carbonyl sulfide (COS) has been recognized as a promising indicator of the plant gross primary production (GPP). Here, we assimilate both COS and CO2 measurements into an atmospheric transport model to obtain information on GPP, plant respiration and COS budget. A possible scenario for the period 2008–2019 leads to a global COS biospheric sink of 800 GgS yr−1 and higher oceanic emissions between 400 and 600 GgS yr−1.
Yanan Zhao, Dennis Booge, Christa A. Marandino, Cathleen Schlundt, Astrid Bracher, Elliot L. Atlas, Jonathan Williams, and Hermann W. Bange
Biogeosciences, 19, 701–714, https://doi.org/10.5194/bg-19-701-2022, https://doi.org/10.5194/bg-19-701-2022, 2022
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We present here, for the first time, simultaneously measured dimethylsulfide (DMS) seawater concentrations and DMS atmospheric mole fractions from the Peruvian upwelling region during two cruises in December 2012 and October 2015. Our results indicate low oceanic DMS concentrations and atmospheric DMS molar fractions in surface waters and the atmosphere, respectively. In addition, the Peruvian upwelling region was identified as an insignificant source of DMS emissions during both periods.
Clara M. Nussbaumer, John N. Crowley, Jan Schuladen, Jonathan Williams, Sascha Hafermann, Andreas Reiffs, Raoul Axinte, Hartwig Harder, Cheryl Ernest, Anna Novelli, Katrin Sala, Monica Martinez, Chinmay Mallik, Laura Tomsche, Christian Plass-Dülmer, Birger Bohn, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 18413–18432, https://doi.org/10.5194/acp-21-18413-2021, https://doi.org/10.5194/acp-21-18413-2021, 2021
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HCHO is an important atmospheric trace gas influencing the photochemical processes in the Earth’s atmosphere, including the budget of HOx and the abundance of tropospheric O3. This research presents the photochemical calculations of HCHO and O3 based on three field campaigns across Europe. We show that HCHO production via the oxidation of only four volatile organic compound precursors, i.e., CH4, CH3CHO, C5H8 and CH3OH, can balance the observed loss at all sites well.
Dirk Dienhart, John N. Crowley, Efstratios Bourtsoukidis, Achim Edtbauer, Philipp G. Eger, Lisa Ernle, Hartwig Harder, Bettina Hottmann, Monica Martinez, Uwe Parchatka, Jean-Daniel Paris, Eva Y. Pfannerstill, Roland Rohloff, Jan Schuladen, Christof Stönner, Ivan Tadic, Sebastian Tauer, Nijing Wang, Jonathan Williams, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 17373–17388, https://doi.org/10.5194/acp-21-17373-2021, https://doi.org/10.5194/acp-21-17373-2021, 2021
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We present the first ship-based in situ measurements of formaldehyde (HCHO), hydroxyl radicals (OH) and the OH reactivity around the Arabian Peninsula. Regression analysis of the HCHO production rate and the related OH chemistry revealed the regional HCHO yield αeff, which represents the different chemical regimes encountered. Highest values were found for the Arabian Gulf (also known as the Persian Gulf), which highlights this region as a hotspot of photochemical air pollution.
Clara M. Nussbaumer, Uwe Parchatka, Ivan Tadic, Birger Bohn, Daniel Marno, Monica Martinez, Roland Rohloff, Hartwig Harder, Flora Kluge, Klaus Pfeilsticker, Florian Obersteiner, Martin Zöger, Raphael Doerich, John N. Crowley, Jos Lelieveld, and Horst Fischer
Atmos. Meas. Tech., 14, 6759–6776, https://doi.org/10.5194/amt-14-6759-2021, https://doi.org/10.5194/amt-14-6759-2021, 2021
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NO2 plays a central role in atmospheric photochemical processes and requires accurate measurements. This research presents NO2 data obtained via chemiluminescence using a photolytic converter from airborne studies around Cabo Verde and laboratory investigations. We show the limits and error-proneness of a conventional blue light converter in aircraft measurements affected by humidity and NO levels and suggest the use of an alternative quartz converter for more reliable results.
Vlassis A. Karydis, Alexandra P. Tsimpidi, Andrea Pozzer, and Jos Lelieveld
Atmos. Chem. Phys., 21, 14983–15001, https://doi.org/10.5194/acp-21-14983-2021, https://doi.org/10.5194/acp-21-14983-2021, 2021
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Aerosol particle pH is well-buffered by alkaline compounds, notably NH3 and crustal elements. NH3 is found to supply remarkable buffering capacity on a global scale, from the polluted continents to the remote oceans. Potential future changes in agricultural NH3 must be accompanied by strong reductions of SO2 and NOx to avoid particles becoming highly acidic, with implications for human health (aerosol toxicity), ecosystems (acid deposition), clouds, and climate (aerosol hygroscopicity).
Philipp G. Eger, Luc Vereecken, Rolf Sander, Jan Schuladen, Nicolas Sobanski, Horst Fischer, Einar Karu, Jonathan Williams, Ville Vakkari, Tuukka Petäjä, Jos Lelieveld, Andrea Pozzer, and John N. Crowley
Atmos. Chem. Phys., 21, 14333–14349, https://doi.org/10.5194/acp-21-14333-2021, https://doi.org/10.5194/acp-21-14333-2021, 2021
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We determine the impact of pyruvic acid photolysis on the formation of acetaldehyde and peroxy radicals during summer and autumn in the Finnish boreal forest using a data-constrained box model. Our results are dependent on the chosen scenario in which the overall quantum yield and the photolysis products are varied. We highlight that pyruvic acid photolysis can be an important contributor to acetaldehyde and peroxy radical formation in remote, forested regions.
Antoine Berchet, Espen Sollum, Rona L. Thompson, Isabelle Pison, Joël Thanwerdas, Grégoire Broquet, Frédéric Chevallier, Tuula Aalto, Adrien Berchet, Peter Bergamaschi, Dominik Brunner, Richard Engelen, Audrey Fortems-Cheiney, Christoph Gerbig, Christine D. Groot Zwaaftink, Jean-Matthieu Haussaire, Stephan Henne, Sander Houweling, Ute Karstens, Werner L. Kutsch, Ingrid T. Luijkx, Guillaume Monteil, Paul I. Palmer, Jacob C. A. van Peet, Wouter Peters, Philippe Peylin, Elise Potier, Christian Rödenbeck, Marielle Saunois, Marko Scholze, Aki Tsuruta, and Yuanhong Zhao
Geosci. Model Dev., 14, 5331–5354, https://doi.org/10.5194/gmd-14-5331-2021, https://doi.org/10.5194/gmd-14-5331-2021, 2021
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We present here the Community Inversion Framework (CIF) to help rationalize development efforts and leverage the strengths of individual inversion systems into a comprehensive framework. The CIF is a programming protocol to allow various inversion bricks to be exchanged among researchers.
The ensemble of bricks makes a flexible, transparent and open-source Python-based tool. We describe the main structure and functionalities and demonstrate it in a simple academic case.
James Weber, Scott Archer-Nicholls, Nathan Luke Abraham, Youngsub M. Shin, Thomas J. Bannan, Carl J. Percival, Asan Bacak, Paulo Artaxo, Michael Jenkin, M. Anwar H. Khan, Dudley E. Shallcross, Rebecca H. Schwantes, Jonathan Williams, and Alex T. Archibald
Geosci. Model Dev., 14, 5239–5268, https://doi.org/10.5194/gmd-14-5239-2021, https://doi.org/10.5194/gmd-14-5239-2021, 2021
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The new mechanism CRI-Strat 2 features state-of-the-art isoprene chemistry not previously available in UKCA and improves UKCA's ability to reproduce observed concentrations of isoprene, monoterpenes, and OH in tropical regions. The enhanced ability to model isoprene, the most widely emitted non-methane volatile organic compound (VOC), will allow understanding of how isoprene and other biogenic VOCs affect atmospheric composition and, through biosphere–atmosphere feedbacks, climate change.
Patrick Dewald, Raphael Dörich, Jan Schuladen, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 14, 5501–5519, https://doi.org/10.5194/amt-14-5501-2021, https://doi.org/10.5194/amt-14-5501-2021, 2021
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Organic nitrates generated from the reaction between isoprene and the nitrate radical (ISOP-NITs) were detected via their thermal dissociation in heated quartz inlets to nitrogen dioxide monitored by cavity ring-down spectroscopy. The temperature-dependent dissociation profiles of ISOP-NITs in the presence of ozone (O3) are broad in contrast to narrow profiles of common reference compounds. We demonstrate that this broadening is caused by O3-assisted reactions of ISOP-NITs on quartz surfaces.
Raphael Dörich, Philipp Eger, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 14, 5319–5332, https://doi.org/10.5194/amt-14-5319-2021, https://doi.org/10.5194/amt-14-5319-2021, 2021
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We demonstrate in laboratory experiments that the formation of IOx anions (formed in reactions of I− with O3) or acetate anions (formed e.g. by the reaction of I− with peracetic acid) results in unexpected sensitivity of an iodide chemical ionisation mass spectrometer (I-CIMS) to HNO3 at a mass-to-charge ratio of 62. This helps explain observations of apparent high daytime levels of N2O5. Airborne measurements using I-CIMS confirm these conclusions.
Vinod Kumar, Julia Remmers, Steffen Beirle, Joachim Fallmann, Astrid Kerkweg, Jos Lelieveld, Mariano Mertens, Andrea Pozzer, Benedikt Steil, Marc Barra, Holger Tost, and Thomas Wagner
Atmos. Meas. Tech., 14, 5241–5269, https://doi.org/10.5194/amt-14-5241-2021, https://doi.org/10.5194/amt-14-5241-2021, 2021
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We present high-resolution regional atmospheric chemistry model simulations focused around Germany. We highlight the importance of spatial resolution of the model itself as well as the input emissions inventory and short-scale temporal variability of emissions for simulations. We propose a consistent approach for evaluating the simulated vertical distribution of NO2 using MAX-DOAS measurements while also considering its spatial sensitivity volume and change in sensitivity within this volume.
Sara M. Defratyka, Jean-Daniel Paris, Camille Yver-Kwok, Daniel Loeb, James France, Jon Helmore, Nigel Yarrow, Valérie Gros, and Philippe Bousquet
Atmos. Meas. Tech., 14, 5049–5069, https://doi.org/10.5194/amt-14-5049-2021, https://doi.org/10.5194/amt-14-5049-2021, 2021
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We consider the possibility of using the CRDS Picarro G2201-i instrument, originally designed for isotopic CH4 and CO2, for measurements of ethane : methane in near-source conditions. The work involved laboratory tests, a controlled release experiment and mobile measurements. We show the potential of determining ethane : methane with 50 ppb ethane uncertainty. The instrument can correctly estimate the ratio in CH4 enhancements of 1 ppm and more, as can be found at strongly emitting sites.
Klaus Klingmüller and Jos Lelieveld
Geosci. Model Dev., 14, 4429–4441, https://doi.org/10.5194/gmd-14-4429-2021, https://doi.org/10.5194/gmd-14-4429-2021, 2021
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Soil moisture is of great importance for weather and climate. We present a machine learning model that produces accurate predictions of satellite-observed surface soil moisture, based on meteorological data from a climate model. It can be used as soil moisture parametrisation in climate models and to produce comprehensive global soil moisture datasets. Moreover, it may motivate similar applications of machine learning in climate science.
Ivan Tadic, Clara M. Nussbaumer, Birger Bohn, Hartwig Harder, Daniel Marno, Monica Martinez, Florian Obersteiner, Uwe Parchatka, Andrea Pozzer, Roland Rohloff, Martin Zöger, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 8195–8211, https://doi.org/10.5194/acp-21-8195-2021, https://doi.org/10.5194/acp-21-8195-2021, 2021
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Although mechanisms of tropospheric ozone (O3) formation are well understood, studies reporting on ozone formation derived from field measurements are challenging and remain sparse in number. We use airborne measurements to quantify nitric oxide (NO) and O3 distributions in the upper troposphere over the Atlantic Ocean and western Africa and compare our measurements to model simulations. Our results show that NO and ozone formation are greatest over the tropical areas of western Africa.
Audrey Fortems-Cheiney, Isabelle Pison, Grégoire Broquet, Gaëlle Dufour, Antoine Berchet, Elise Potier, Adriana Coman, Guillaume Siour, and Lorenzo Costantino
Geosci. Model Dev., 14, 2939–2957, https://doi.org/10.5194/gmd-14-2939-2021, https://doi.org/10.5194/gmd-14-2939-2021, 2021
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Up-to-date and accurate emission inventories for air pollutants are essential for understanding their role in the formation of tropospheric ozone and particulate matter, for anticipating pollution peaks and for identifying the key drivers that could help mitigate their emissions. Complementarily with bottom-up inventories, the system described here aims at updating and improving the knowledge on the high spatiotemporal variability of emissions of air pollutants.
Clara M. Nussbaumer, Ivan Tadic, Dirk Dienhart, Nijing Wang, Achim Edtbauer, Lisa Ernle, Jonathan Williams, Florian Obersteiner, Isidoro Gutiérrez-Álvarez, Hartwig Harder, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 7933–7945, https://doi.org/10.5194/acp-21-7933-2021, https://doi.org/10.5194/acp-21-7933-2021, 2021
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Lightning over continental and coastal areas is frequent and accompanied by deep convection, while lightning over marine areas and particularly in tropical cyclones is rare. This research presents in situ observations of the tropical storm Florence 2018 near Cabo Verde. We show the absence of lightning in the tropical storm despite the occurrence of deep convective processes by atmospheric trace gas measurements of O3, NO, CO, H2O2, DMS and CH2I.
Nils Friedrich, Philipp Eger, Justin Shenolikar, Nicolas Sobanski, Jan Schuladen, Dirk Dienhart, Bettina Hottmann, Ivan Tadic, Horst Fischer, Monica Martinez, Roland Rohloff, Sebastian Tauer, Hartwig Harder, Eva Y. Pfannerstill, Nijing Wang, Jonathan Williams, James Brooks, Frank Drewnick, Hang Su, Guo Li, Yafang Cheng, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 21, 7473–7498, https://doi.org/10.5194/acp-21-7473-2021, https://doi.org/10.5194/acp-21-7473-2021, 2021
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This paper uses NOx and NOz measurements from the 2017 AQABA ship campaign in the Mediterranean Sea and around the Arabian Peninsula to examine the influence e.g. of emissions from shipping and oil and gas production. Night-time losses of NOx dominated in the Arabian Gulf and in the Red Sea, whereas daytime losses were more important in the Mediterranean Sea. Nitric acid and organic nitrates were the most prevalent components of NOz.
Eva Y. Pfannerstill, Nina G. Reijrink, Achim Edtbauer, Akima Ringsdorf, Nora Zannoni, Alessandro Araújo, Florian Ditas, Bruna A. Holanda, Marta O. Sá, Anywhere Tsokankunku, David Walter, Stefan Wolff, Jošt V. Lavrič, Christopher Pöhlker, Matthias Sörgel, and Jonathan Williams
Atmos. Chem. Phys., 21, 6231–6256, https://doi.org/10.5194/acp-21-6231-2021, https://doi.org/10.5194/acp-21-6231-2021, 2021
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Tropical forests are globally significant for atmospheric chemistry. However, the mixture of reactive organic gases emitted by these ecosystems is poorly understood. By comprehensive observations at an Amazon forest site, we show that oxygenated species were previously underestimated in their contribution to the tropical-forest reactant mix. Our results show rain and temperature effects and have implications for models and the understanding of ozone and particle formation above tropical forests.
Wenjie Wang, Jipeng Qi, Jun Zhou, Bin Yuan, Yuwen Peng, Sihang Wang, Suxia Yang, Jonathan Williams, Vinayak Sinha, and Min Shao
Atmos. Meas. Tech., 14, 2285–2298, https://doi.org/10.5194/amt-14-2285-2021, https://doi.org/10.5194/amt-14-2285-2021, 2021
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We designed a new reactor for measurements of OH reactivity (i.e., OH radical loss frequency) based on the comparative reactivity method under
high-NOx conditions, such as in cities. We performed a series of laboratory tests to evaluate the new reactor. The new reactor was used in the field and performed well in measuring OH reactivity in air influenced by upwind cities.
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.
Domenico Taraborrelli, David Cabrera-Perez, Sara Bacer, Sergey Gromov, Jos Lelieveld, Rolf Sander, and Andrea Pozzer
Atmos. Chem. Phys., 21, 2615–2636, https://doi.org/10.5194/acp-21-2615-2021, https://doi.org/10.5194/acp-21-2615-2021, 2021
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Atmospheric pollutants from anthropogenic activities and biomass burning are usually regarded as ozone precursors. Monocyclic aromatics are no exception. Calculations with a comprehensive atmospheric model are consistent with this view but only for air masses close to pollution source regions. However, the same model predicts that aromatics, when transported to remote areas, may effectively destroy ozone. This loss of tropospheric ozone rivals the one attributed to bromine.
Sara Bacer, Sylvia C. Sullivan, Odran Sourdeval, Holger Tost, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 21, 1485–1505, https://doi.org/10.5194/acp-21-1485-2021, https://doi.org/10.5194/acp-21-1485-2021, 2021
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We investigate the relative importance of the rates of both microphysical processes and unphysical correction terms that act as sources or sinks of ice crystals in cold clouds. By means of numerical simulations performed with a global chemistry–climate model, we assess the relevance of these rates at global and regional scales. This estimation is of fundamental importance to assign priority to the development of microphysics parameterizations and compare model output with observations.
Camille Yver-Kwok, Carole Philippon, Peter Bergamaschi, Tobias Biermann, Francescopiero Calzolari, Huilin Chen, Sebastien Conil, Paolo Cristofanelli, Marc Delmotte, Juha Hatakka, Michal Heliasz, Ove Hermansen, Kateřina Komínková, Dagmar Kubistin, Nicolas Kumps, Olivier Laurent, Tuomas Laurila, Irene Lehner, Janne Levula, Matthias Lindauer, Morgan Lopez, Ivan Mammarella, Giovanni Manca, Per Marklund, Jean-Marc Metzger, Meelis Mölder, Stephen M. Platt, Michel Ramonet, Leonard Rivier, Bert Scheeren, Mahesh Kumar Sha, Paul Smith, Martin Steinbacher, Gabriela Vítková, and Simon Wyss
Atmos. Meas. Tech., 14, 89–116, https://doi.org/10.5194/amt-14-89-2021, https://doi.org/10.5194/amt-14-89-2021, 2021
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The Integrated Carbon Observation System (ICOS) is a pan-European research infrastructure which provides harmonized and high-precision scientific data on the carbon cycle and the greenhouse gas (GHG) budget. All stations have to undergo a rigorous assessment before being labeled, i.e., receiving approval to join the network. In this paper, we present the labeling process for the ICOS atmospheric network through the 23 stations that were labeled between November 2017 and November 2019.
Klaus Klingmüller, Vlassis A. Karydis, Sara Bacer, Georgiy L. Stenchikov, and Jos Lelieveld
Atmos. Chem. Phys., 20, 15285–15295, https://doi.org/10.5194/acp-20-15285-2020, https://doi.org/10.5194/acp-20-15285-2020, 2020
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Particulate air pollution cools the climate and partially masks the greenhouse warming by reflecting sunlight and enhancing the reflection by clouds. The intensity of this cooling depends on interactions between pollution and desert dust within the atmosphere. Our simulations with a global atmospheric chemistry-climate model indicate that these interactions significantly weaken the cooling.
Matias Berasategui, Damien Amedro, Luc Vereecken, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 13541–13555, https://doi.org/10.5194/acp-20-13541-2020, https://doi.org/10.5194/acp-20-13541-2020, 2020
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Peracetic acid is one of the most abundant organic peroxides in the atmosphere. We combine experiments and theory to show that peracetic acid reacts orders of magnitude more slowly with OH than presently accepted, which results in a significant extension of its atmospheric lifetime.
Yuanhong Zhao, Marielle Saunois, Philippe Bousquet, Xin Lin, Antoine Berchet, Michaela I. Hegglin, Josep G. Canadell, Robert B. Jackson, Makoto Deushi, Patrick Jöckel, Douglas Kinnison, Ole Kirner, Sarah Strode, Simone Tilmes, Edward J. Dlugokencky, and Bo Zheng
Atmos. Chem. Phys., 20, 13011–13022, https://doi.org/10.5194/acp-20-13011-2020, https://doi.org/10.5194/acp-20-13011-2020, 2020
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Decadal trends and variations in OH are critical for understanding atmospheric CH4 evolution. We quantify the impacts of OH trends and variations on the CH4 budget by conducting CH4 inversions on a decadal scale with an ensemble of OH fields. We find the negative OH anomalies due to enhanced fires can reduce the optimized CH4 emissions by up to 10 Tg yr−1 during El Niño years and the positive OH trend from 1986 to 2010 results in a ∼ 23 Tg yr−1 additional increase in optimized CH4 emissions.
Bettina Hottmann, Sascha Hafermann, Laura Tomsche, Daniel Marno, Monica Martinez, Hartwig Harder, Andrea Pozzer, Marco Neumaier, Andreas Zahn, Birger Bohn, Greta Stratmann, Helmut Ziereis, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 20, 12655–12673, https://doi.org/10.5194/acp-20-12655-2020, https://doi.org/10.5194/acp-20-12655-2020, 2020
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During OMO we observed enhanced mixing ratios of hydroperoxides (ROOH) in the Asian monsoon anticyclone (AMA) relative to the background. The observed mixing ratios are higher than steady-state calculations and EMAC simulations, especially in the AMA, indicating atmospheric transport of ROOH. Uncertainties in the scavenging efficiencies likely cause deviations from EMAC. Longitudinal gradients indicate a pool of ROOH towards the center of the AMA associated with upwind convection over India.
Nils Friedrich, Ivan Tadic, Jan Schuladen, James Brooks, Eoghan Darbyshire, Frank Drewnick, Horst Fischer, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 13, 5739–5761, https://doi.org/10.5194/amt-13-5739-2020, https://doi.org/10.5194/amt-13-5739-2020, 2020
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We present a new instrument for the measurement of NOx and NOy based on a combination of the thermal dissociation of NOy to NOx and cavity ring-down spectroscopic detection of NO2. It features a denuder to separate the contributions of gas-phase and particulate nitrates to NOy. We provide a detailed characterization of the instrument and briefly outline results from first deployments.
Nijing Wang, Achim Edtbauer, Christof Stönner, Andrea Pozzer, Efstratios Bourtsoukidis, Lisa Ernle, Dirk Dienhart, Bettina Hottmann, Horst Fischer, Jan Schuladen, John N. Crowley, Jean-Daniel Paris, Jos Lelieveld, and Jonathan Williams
Atmos. Chem. Phys., 20, 10807–10829, https://doi.org/10.5194/acp-20-10807-2020, https://doi.org/10.5194/acp-20-10807-2020, 2020
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Carbonyl compounds were measured on a ship travelling around the Arabian Peninsula in summer 2017, crossing both highly polluted and extremely clean regions of the marine boundary layer. We investigated the sources and sinks of carbonyls. The results from a global model showed a significant model underestimation for acetaldehyde, a molecule that can influence regional air chemistry. By adding a diurnal oceanic source, the model estimation was highly improved.
Patrick Dewald, Jonathan M. Liebmann, Nils Friedrich, Justin Shenolikar, Jan Schuladen, Franz Rohrer, David Reimer, Ralf Tillmann, Anna Novelli, Changmin Cho, Kangming Xu, Rupert Holzinger, François Bernard, Li Zhou, Wahid Mellouki, Steven S. Brown, Hendrik Fuchs, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 10459–10475, https://doi.org/10.5194/acp-20-10459-2020, https://doi.org/10.5194/acp-20-10459-2020, 2020
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We present direct measurements of NO3 reactivity resulting from the oxidation of isoprene by NO3 during an intensive simulation chamber study. Measurements were in excellent agreement with values calculated from measured isoprene amounts and the rate coefficient for the reaction of NO3 with isoprene. Comparison of the measurement with NO3 reactivities from non-steady-state and model calculations suggests that isoprene-derived RO2 and HO2 radicals account to ~ 50 % of overall NO3 losses.
Cited articles
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Kort, E. A., Lamb, B. K., Lauvaux, T., Maasakkers, J. D., Marchese, A. J.,
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Berchet, A., Pison, I., Crill, P. M., Thornton, B., Bousquet, P., Thonat, T., Hocking, T., Thanwerdas, J., Paris, J.-D., and Saunois, M.: Using ship-borne observations of methane isotopic ratio in the Arctic Ocean to understand methane sources in the Arctic, Atmos. Chem. Phys., 20, 3987–3998, https://doi.org/10.5194/acp-20-3987-2020, 2020.
Bourtsoukidis, E., Ernle, L., Crowley, J. N., Lelieveld, J., Paris, J.-D., Pozzer, A., Walter, D., and Williams, J.: Non-methane hydrocarbon (C2–C8) sources and sinks around the Arabian Peninsula, Atmos. Chem. Phys., 19, 7209–7232, https://doi.org/10.5194/acp-19-7209-2019, 2019.
Bourtsoukidis, E., Pozzer, A., Sattler, T., Matthaios, V. N., Ernle, L.,
Edtbauer, A., Fischer, H., Könemann, T., Osipov, S., Paris, J.-D.,
Pfannerstill, E. Y., Stönner, C., Tadic, I., Walter, D., Wang, N., Lelieveld, J., and Williams, J.: The Red Sea Deep Water is a potent source of atmospheric ethane and propane, Nat. Commun., 11, 447,
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Short summary
We measured atmospheric methane and CO2 by ship in the Middle East. We probe the origin of methane with a combination of light alkane measurements and modeling. We find strong influence from nearby oil and gas production over the Arabian Gulf. Comparing our data to inventories indicates that inventories overestimate sources from the upstream gas industry but underestimate emissions from oil extraction and processing. The Red Sea was under a complex mixture of sources due to human activity.
We measured atmospheric methane and CO2 by ship in the Middle East. We probe the origin of...
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