Articles | Volume 13, issue 4
https://doi.org/10.5194/acp-13-2267-2013
© Author(s) 2013. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-13-2267-2013
© Author(s) 2013. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
27 Feb 2013
Research article |
| 27 Feb 2013
Analysis of global methane changes after the 1991 Pinatubo volcanic eruption
N. Bândă
Institute for Marine and Atmospheric Research Utrecht, Utrecht University, Utrecht, The Netherlands
Royal Netherlands Meteorological Institute (KNMI), De Bilt, The Netherlands
Institute for Marine and Atmospheric Research Utrecht, Utrecht University, Utrecht, The Netherlands
Dept. of Meteorology and Air Quality, Wageningen University and Research Center, Wageningen, The Netherlands
Netherlands Institute for Space Research (SRON), Utrecht, The Netherlands
M. van Weele
Royal Netherlands Meteorological Institute (KNMI), De Bilt, The Netherlands
T. van Noije
Royal Netherlands Meteorological Institute (KNMI), De Bilt, The Netherlands
T. Röckmann
Institute for Marine and Atmospheric Research Utrecht, Utrecht University, Utrecht, The Netherlands
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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
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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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.
Alba Mols, Klaas Folkert Boersma, Hugo Denier van der Gon, and Maarten Krol
EGUsphere, https://doi.org/10.5194/egusphere-2025-49, https://doi.org/10.5194/egusphere-2025-49, 2025
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We created a new method to estimate city air pollution (NOx emissions) using satellite data. Testing showed our approach works well to track how pollution spreads in urban areas. By combining observations with prior knowledge, we improved the accuracy of emission estimates. Applying this method in Paris, we found emissions were 9 % lower than expected and dropped significantly during COVID-19 lockdowns. Our method offers a reliable way to monitor pollution and support environmental policies.
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
EGUsphere, https://doi.org/10.5194/egusphere-2024-3620, https://doi.org/10.5194/egusphere-2024-3620, 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 analyzers when they transect 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.
Gerrit Kuhlmann, Foteini Stavropoulou, Stefan Schwietzke, Daniel Zavala-Araiza, Andrew Thorpe, Andreas Hueni, Lukas Emmenegger, Andreea Calcan, Thomas Röckmann, and Dominik Brunner
EGUsphere, https://doi.org/10.5194/egusphere-2024-3494, https://doi.org/10.5194/egusphere-2024-3494, 2024
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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.
Getachew Agmuas Adnew, Gerbrand Koren, Neha Mehendale, Sergey Gromov, Maarten Krol, and Thomas Röckmann
EGUsphere, https://doi.org/10.5194/egusphere-2024-3231, https://doi.org/10.5194/egusphere-2024-3231, 2024
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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.
Manu Anna Thomas, Klaus Wyser, Shiyu Wang, Marios Chatziparaschos, Paraskevi Georgakaki, Montserrat Costa-Surós, Maria Gonçalves Ageitos, Maria Kanakidou, Carlos Pérez García-Pando, Athanasios Nenes, Twan van Noije, Philippe Le Sager, and Abhay Devasthale
Geosci. Model Dev., 17, 6903–6927, https://doi.org/10.5194/gmd-17-6903-2024, https://doi.org/10.5194/gmd-17-6903-2024, 2024
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Aerosol–cloud interactions occur at a range of spatio-temporal scales. While evaluating recent developments in EC-Earth3-AerChem, this study aims to understand the extent to which the Twomey effect manifests itself at larger scales. We find a reduction in the warm bias over the Southern Ocean due to model improvements. While we see footprints of the Twomey effect at larger scales, the negative relationship between cloud droplet number and liquid water drives the shortwave radiative effect.
Maarten Krol, Bart van Stratum, Isidora Anglou, and Klaas Folkert Boersma
Atmos. Chem. Phys., 24, 8243–8262, https://doi.org/10.5194/acp-24-8243-2024, https://doi.org/10.5194/acp-24-8243-2024, 2024
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This paper presents detailed plume simulations of nitrogen oxides and carbon dioxide that are emitted from four large industrial facilities world-wide. Results from the high-resolution simulations that include atmospheric chemistry are compared to nitrogen dioxide observations from satellites. We find good performance of the model and show that common assumptions that are used in simplified models need revision. This work is important for the monitoring of emissions using satellite data.
Alkiviadis Kalisoras, Aristeidis K. Georgoulias, Dimitris Akritidis, Robert J. Allen, Vaishali Naik, Chaincy Kuo, Sophie Szopa, Pierre Nabat, Dirk Olivié, Twan van Noije, Philippe Le Sager, David Neubauer, Naga Oshima, Jane Mulcahy, Larry W. Horowitz, and Prodromos Zanis
Atmos. Chem. Phys., 24, 7837–7872, https://doi.org/10.5194/acp-24-7837-2024, https://doi.org/10.5194/acp-24-7837-2024, 2024
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Effective radiative forcing (ERF) is a metric for estimating how human activities and natural agents change the energy flow into and out of the Earth’s climate system. We investigate the anthropogenic aerosol ERF, and we estimate the contribution of individual processes to the total ERF using simulations from Earth system models within the Coupled Model Intercomparison Project Phase 6 (CMIP6). Our findings highlight that aerosol–cloud interactions drive ERF variability during the last 150 years.
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.
Johann Rasmus Nüß, Nikos Daskalakis, Fabian Günther Piwowarczyk, Angelos Gkouvousis, Oliver Schneising, Michael Buchwitz, Maria Kanakidou, Maarten C. Krol, and Mihalis Vrekoussis
EGUsphere, https://doi.org/10.5194/egusphere-2024-1595, https://doi.org/10.5194/egusphere-2024-1595, 2024
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We estimate carbon monoxide emissions through inverse modeling, an approach where measurements of tracers in the atmosphere are fed into a model to calculate backwards in time (inverse) where the tracers came from. We introduce measurements from a new satellite instrument and show that, in most places globally, these on their own sufficiently constrain the emissions. This alleviates the need for additional datasets, which could shorten the delay for future carbon monoxide source estimates.
Sandro Meier, Erik F. M. Koene, Maarten Krol, Dominik Brunner, Alexander Damm, and Gerrit Kuhlmann
Atmos. Chem. Phys., 24, 7667–7686, https://doi.org/10.5194/acp-24-7667-2024, https://doi.org/10.5194/acp-24-7667-2024, 2024
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Nitrogen oxides (NOx = NO + NO2) are important air pollutants. This study addresses the challenge of accurately estimating NOx emissions from NO2 satellite observations. We develop a realistic model to convert NO2 to NOx by using simulated plumes from various power plants. We apply the model to satellite NO2 observations, significantly reducing biases in estimated NOx emissions. The study highlights the potential for a consistent, high-resolution estimation of NOx emissions using satellite data.
Fangxuan Ren, Jintai Lin, Chenghao Xu, Jamiu A. Adeniran, Jingxu Wang, Randall V. Martin, Aaron van Donkelaar, Melanie S. Hammer, Larry W. Horowitz, Steven T. Turnock, Naga Oshima, Jie Zhang, Susanne Bauer, Kostas Tsigaridis, Øyvind Seland, Pierre Nabat, David Neubauer, Gary Strand, Twan van Noije, Philippe Le Sager, and Toshihiko Takemura
Geosci. Model Dev., 17, 4821–4836, https://doi.org/10.5194/gmd-17-4821-2024, https://doi.org/10.5194/gmd-17-4821-2024, 2024
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We evaluate the performance of 14 CMIP6 ESMs in simulating total PM2.5 and its 5 components over China during 2000–2014. PM2.5 and its components are underestimated in almost all models, except that black carbon (BC) and sulfate are overestimated in two models, respectively. The underestimation is the largest for organic carbon (OC) and the smallest for BC. Models reproduce the observed spatial pattern for OC, sulfate, nitrate and ammonium well, yet the agreement is poorer for BC.
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.
Malavika Sivan, Thomas Röckmann, Carina van der Veen, and Maria Elena Popa
Atmos. Meas. Tech., 17, 2687–2705, https://doi.org/10.5194/amt-17-2687-2024, https://doi.org/10.5194/amt-17-2687-2024, 2024
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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.
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.
Putian Zhou, Zhengyao Lu, Jukka-Pekka Keskinen, Qiong Zhang, Juha Lento, Jianpu Bian, Twan van Noije, Philippe Le Sager, Veli-Matti Kerminen, Markku Kulmala, Michael Boy, and Risto Makkonen
Clim. Past, 19, 2445–2462, https://doi.org/10.5194/cp-19-2445-2023, https://doi.org/10.5194/cp-19-2445-2023, 2023
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A Green Sahara with enhanced rainfall and larger vegetation cover existed in northern Africa about 6000 years ago. Biosphere–atmosphere interactions are found to be critical to explaining this wet period. Based on modeled vegetation reconstruction data, we simulated dust emissions and aerosol formation, which are key factors in biosphere–atmosphere interactions. Our results also provide a benchmark of aerosol climatology for future paleo-climate simulation experiments.
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.
Farhan R. Nursanto, Roy Meinen, Rupert Holzinger, Maarten C. Krol, Xinya Liu, Ulrike Dusek, Bas Henzing, and Juliane L. Fry
Atmos. Chem. Phys., 23, 10015–10034, https://doi.org/10.5194/acp-23-10015-2023, https://doi.org/10.5194/acp-23-10015-2023, 2023
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Particulate matter (PM) is a harmful air pollutant that depends on the complex mixture of natural and anthropogenic emissions into the atmosphere. Thus, in different regions and seasons, the way that PM is formed and grows can differ. In this study, we use a combined statistical analysis of the chemical composition and particle size distribution to determine what drives particle formation and growth across seasons, using varying wind directions to elucidate the role of different sources.
Alessandro Zanchetta, Linda M. J. Kooijmans, Steven van Heuven, Andrea Scifo, Hubertus A. Scheeren, Ivan Mammarella, Ute Karstens, Jin Ma, Maarten Krol, and Huilin Chen
Biogeosciences, 20, 3539–3553, https://doi.org/10.5194/bg-20-3539-2023, https://doi.org/10.5194/bg-20-3539-2023, 2023
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Carbonyl sulfide (COS) has been suggested as a tool to estimate carbon dioxide (CO2) uptake by plants during photosynthesis. However, understanding its sources and sinks is critical to preventing biases in this estimate. Combining observations and models, this study proves that regional sources occasionally influence the measurements at the 60 m tall Lutjewad tower (1 m a.s.l.; 53°24′ N, 6°21′ E) in the Netherlands. Moreover, it estimates nighttime COS fluxes to be −3.0 ± 2.6 pmol m−2 s−1.
Ara Cho, Linda M. J. Kooijmans, Kukka-Maaria Kohonen, Richard Wehr, and Maarten C. Krol
Biogeosciences, 20, 2573–2594, https://doi.org/10.5194/bg-20-2573-2023, https://doi.org/10.5194/bg-20-2573-2023, 2023
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Carbonyl sulfide (COS) is a useful constraint for estimating photosynthesis. To simulate COS leaf flux better in the SiB4 model, we propose a novel temperature function for enzyme carbonic anhydrase (CA) activity and optimize conductances using observations. The optimal activity of CA occurs below 40 °C, and Ball–Woodrow–Berry parameters are slightly changed. These reduce/increase uptakes in the tropics/higher latitudes and contribute to resolving discrepancies in the COS global budget.
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.
Peter J. M. Bosman and Maarten C. Krol
Geosci. Model Dev., 16, 47–74, https://doi.org/10.5194/gmd-16-47-2023, https://doi.org/10.5194/gmd-16-47-2023, 2023
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We describe an inverse modelling framework constructed around a simple model for the atmospheric boundary layer. This framework can be fed with various observation types to study the boundary layer and land–atmosphere exchange. With this framework, it is possible to estimate model parameters and the associated uncertainties. Some of these parameters are difficult to obtain directly by observations. An example application for a grassland in the Netherlands is included.
Srijana Lama, Sander Houweling, K. Folkert Boersma, Ilse Aben, Hugo A. C. Denier van der Gon, and Maarten C. Krol
Atmos. Chem. Phys., 22, 16053–16071, https://doi.org/10.5194/acp-22-16053-2022, https://doi.org/10.5194/acp-22-16053-2022, 2022
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Hydroxyl radical (OH) is the important chemical species that determines the lifetime of some greenhouse gases and trace gases. OH plays a vital role in air pollution chemistry. OH has a short lifetime and is extremely difficult to measure directly. OH concentrations derived from the chemistry transport model (CTM) have uncertainties of >50 %. Therefore, in this study, OH is derived indirectly using satellite date in urban plumes.
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.
Stijn Naus, Lucas G. Domingues, Maarten Krol, Ingrid T. Luijkx, Luciana V. Gatti, John B. Miller, Emanuel Gloor, Sourish Basu, Caio Correia, Gerbrand Koren, Helen M. Worden, Johannes Flemming, Gabrielle Pétron, and Wouter Peters
Atmos. Chem. Phys., 22, 14735–14750, https://doi.org/10.5194/acp-22-14735-2022, https://doi.org/10.5194/acp-22-14735-2022, 2022
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We assimilate MOPITT CO satellite data in the TM5-4D-Var inverse modelling framework to estimate Amazon fire CO emissions for 2003–2018. We show that fire emissions have decreased over the analysis period, coincident with a decrease in deforestation rates. However, interannual variations in fire emissions are large, and they correlate strongly with soil moisture. Our results reveal an important role for robust, top-down fire CO emissions in quantifying and attributing Amazon fire intensity.
Ville Leinonen, Harri Kokkola, Taina Yli-Juuti, Tero Mielonen, Thomas Kühn, Tuomo Nieminen, Simo Heikkinen, Tuuli Miinalainen, Tommi Bergman, Ken Carslaw, Stefano Decesari, Markus Fiebig, Tareq Hussein, Niku Kivekäs, Radovan Krejci, Markku Kulmala, Ari Leskinen, Andreas Massling, Nikos Mihalopoulos, Jane P. Mulcahy, Steffen M. Noe, Twan van Noije, Fiona M. O'Connor, Colin O'Dowd, Dirk Olivie, Jakob B. Pernov, Tuukka Petäjä, Øyvind Seland, Michael Schulz, Catherine E. Scott, Henrik Skov, Erik Swietlicki, Thomas Tuch, Alfred Wiedensohler, Annele Virtanen, and Santtu Mikkonen
Atmos. Chem. Phys., 22, 12873–12905, https://doi.org/10.5194/acp-22-12873-2022, https://doi.org/10.5194/acp-22-12873-2022, 2022
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We provide the first extensive comparison of detailed aerosol size distribution trends between in situ observations from Europe and five different earth system models. We investigated aerosol modes (nucleation, Aitken, and accumulation) separately and were able to show the differences between measured and modeled trends and especially their seasonal patterns. The differences in model results are likely due to complex effects of several processes instead of certain specific model features.
Malika Menoud, Carina van der Veen, Dave Lowry, Julianne M. Fernandez, Semra Bakkaloglu, James L. France, Rebecca E. Fisher, Hossein Maazallahi, Mila Stanisavljević, Jarosław Nęcki, Katarina Vinkovic, Patryk Łakomiec, Janne Rinne, Piotr Korbeń, Martina Schmidt, Sara Defratyka, Camille Yver-Kwok, Truls Andersen, Huilin Chen, and Thomas Röckmann
Earth Syst. Sci. Data, 14, 4365–4386, https://doi.org/10.5194/essd-14-4365-2022, https://doi.org/10.5194/essd-14-4365-2022, 2022
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Emission sources of methane (CH4) can be distinguished with measurements of CH4 stable isotopes. We present new measurements of isotope signatures of various CH4 sources in Europe, mainly anthropogenic, sampled from 2017 to 2020. The present database also contains the most recent update of the global signature dataset from the literature. The dataset improves CH4 source attribution and the understanding of the global CH4 budget.
Qirui Zhong, Nick Schutgens, Guido van der Werf, Twan van Noije, Kostas Tsigaridis, Susanne E. Bauer, Tero Mielonen, Alf Kirkevåg, Øyvind Seland, Harri Kokkola, Ramiro Checa-Garcia, David Neubauer, Zak Kipling, Hitoshi Matsui, Paul Ginoux, Toshihiko Takemura, Philippe Le Sager, Samuel Rémy, Huisheng Bian, Mian Chin, Kai Zhang, Jialei Zhu, Svetlana G. Tsyro, Gabriele Curci, Anna Protonotariou, Ben Johnson, Joyce E. Penner, Nicolas Bellouin, Ragnhild B. Skeie, and Gunnar Myhre
Atmos. Chem. Phys., 22, 11009–11032, https://doi.org/10.5194/acp-22-11009-2022, https://doi.org/10.5194/acp-22-11009-2022, 2022
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Aerosol optical depth (AOD) errors for biomass burning aerosol (BBA) are evaluated in 18 global models against satellite datasets. Notwithstanding biases in satellite products, they allow model evaluations. We observe large and diverse model biases due to errors in BBA. Further interpretations of AOD diversities suggest large biases exist in key processes for BBA which require better constraining. These results can contribute to further model improvement and development.
Vincent Huijnen, Philippe Le Sager, Marcus O. Köhler, Glenn Carver, Samuel Rémy, Johannes Flemming, Simon Chabrillat, Quentin Errera, and Twan van Noije
Geosci. Model Dev., 15, 6221–6241, https://doi.org/10.5194/gmd-15-6221-2022, https://doi.org/10.5194/gmd-15-6221-2022, 2022
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We report on the first implementation of atmospheric chemistry and aerosol as part of the OpenIFS model, based on the CAMS global model. We give an overview of the model and evaluate two reference model configurations, with and without the stratospheric chemistry extension, against a variety of observational datasets. This OpenIFS version with atmospheric composition components is open to the scientific user community under a standard OpenIFS license.
Anja Ražnjević, Chiel van Heerwaarden, and Maarten Krol
Atmos. Meas. Tech., 15, 3611–3628, https://doi.org/10.5194/amt-15-3611-2022, https://doi.org/10.5194/amt-15-3611-2022, 2022
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We evaluate two widely used observational techniques (Other Test Method (OTM) 33A and car drive-bys) that estimate point source gas emissions. We performed our analysis on high-resolution plume dispersion simulation. For car drive-bys we found that at least 15 repeated measurements were needed to get within 40 % of the true emissions. OTM 33A produced large errors in estimation (50 %–200 %) due to its sensitivity to dispersion coefficients and underlying simplifying assumptions.
Anja Ražnjević, Chiel van Heerwaarden, Bart van Stratum, Arjan Hensen, Ilona Velzeboer, Pim van den Bulk, and Maarten Krol
Atmos. Chem. Phys., 22, 6489–6505, https://doi.org/10.5194/acp-22-6489-2022, https://doi.org/10.5194/acp-22-6489-2022, 2022
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Mobile measurement techniques (e.g., instruments placed in cars) are often employed to identify and quantify individual sources of greenhouse gases. Due to road restrictions, those observations are often sparse (temporally and spatially). We performed high-resolution simulations of plume dispersion, with realistic weather conditions encountered in the field, to reproduce the measurement process of a methane plume emitted from an oil well and provide additional information about the plume.
Ralf Döscher, Mario Acosta, Andrea Alessandri, Peter Anthoni, Thomas Arsouze, Tommi Bergman, Raffaele Bernardello, Souhail Boussetta, Louis-Philippe Caron, Glenn Carver, Miguel Castrillo, Franco Catalano, Ivana Cvijanovic, Paolo Davini, Evelien Dekker, Francisco J. Doblas-Reyes, David Docquier, Pablo Echevarria, Uwe Fladrich, Ramon Fuentes-Franco, Matthias Gröger, Jost v. Hardenberg, Jenny Hieronymus, M. Pasha Karami, Jukka-Pekka Keskinen, Torben Koenigk, Risto Makkonen, François Massonnet, Martin Ménégoz, Paul A. Miller, Eduardo Moreno-Chamarro, Lars Nieradzik, Twan van Noije, Paul Nolan, Declan O'Donnell, Pirkka Ollinaho, Gijs van den Oord, Pablo Ortega, Oriol Tintó Prims, Arthur Ramos, Thomas Reerink, Clement Rousset, Yohan Ruprich-Robert, Philippe Le Sager, Torben Schmith, Roland Schrödner, Federico Serva, Valentina Sicardi, Marianne Sloth Madsen, Benjamin Smith, Tian Tian, Etienne Tourigny, Petteri Uotila, Martin Vancoppenolle, Shiyu Wang, David Wårlind, Ulrika Willén, Klaus Wyser, Shuting Yang, Xavier Yepes-Arbós, and Qiong Zhang
Geosci. Model Dev., 15, 2973–3020, https://doi.org/10.5194/gmd-15-2973-2022, https://doi.org/10.5194/gmd-15-2973-2022, 2022
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The Earth system model EC-Earth3 is documented here. Key performance metrics show physical behavior and biases well within the frame known from recent models. With improved physical and dynamic features, new ESM components, community tools, and largely improved physical performance compared to the CMIP5 version, EC-Earth3 represents a clear step forward for the only European community ESM. We demonstrate here that EC-Earth3 is suited for a range of tasks in CMIP6 and beyond.
Stelios Myriokefalitakis, Elisa Bergas-Massó, María Gonçalves-Ageitos, Carlos Pérez García-Pando, Twan van Noije, Philippe Le Sager, Akinori Ito, Eleni Athanasopoulou, Athanasios Nenes, Maria Kanakidou, Maarten C. Krol, and Evangelos Gerasopoulos
Geosci. Model Dev., 15, 3079–3120, https://doi.org/10.5194/gmd-15-3079-2022, https://doi.org/10.5194/gmd-15-3079-2022, 2022
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We here describe the implementation of atmospheric multiphase processes in the EC-Earth Earth system model. We provide global budgets of oxalate, sulfate, and iron-containing aerosols, along with an analysis of the links among atmospheric composition, aqueous-phase processes, and aerosol dissolution, supported by comparison to observations. This work is a first step towards an interactive calculation of the deposition of bioavailable atmospheric iron coupled to the model’s ocean component.
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.
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.
Tommi Bergman, Risto Makkonen, Roland Schrödner, Erik Swietlicki, Vaughan T. J. Phillips, Philippe Le Sager, and Twan van Noije
Geosci. Model Dev., 15, 683–713, https://doi.org/10.5194/gmd-15-683-2022, https://doi.org/10.5194/gmd-15-683-2022, 2022
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We describe in this paper the implementation of a process-based secondary organic aerosol and new particle formation scheme within the chemistry transport model TM5-MP version 1.2. The performance of the model simulations for the year 2010 is evaluated against in situ observations, ground-based remote sensing and satellite retrievals. Overall, the simulated aerosol fields are improved, although in some areas the model shows a decline in performance.
Linda M. J. Kooijmans, Ara Cho, Jin Ma, Aleya Kaushik, Katherine D. Haynes, Ian Baker, Ingrid T. Luijkx, Mathijs Groenink, Wouter Peters, John B. Miller, Joseph A. Berry, Jerome Ogée, Laura K. Meredith, Wu Sun, Kukka-Maaria Kohonen, Timo Vesala, Ivan Mammarella, Huilin Chen, Felix M. Spielmann, Georg Wohlfahrt, Max Berkelhammer, Mary E. Whelan, Kadmiel Maseyk, Ulli Seibt, Roisin Commane, Richard Wehr, and Maarten Krol
Biogeosciences, 18, 6547–6565, https://doi.org/10.5194/bg-18-6547-2021, https://doi.org/10.5194/bg-18-6547-2021, 2021
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The gas carbonyl sulfide (COS) can be used to estimate photosynthesis. To adopt this approach on regional and global scales, we need biosphere models that can simulate COS exchange. So far, such models have not been evaluated against observations. We evaluate the COS biosphere exchange of the SiB4 model against COS flux observations. We find that the model is capable of simulating key processes in COS biosphere exchange. Still, we give recommendations for further improvement of the model.
Auke J. Visser, Laurens N. Ganzeveld, Ignacio Goded, Maarten C. Krol, Ivan Mammarella, Giovanni Manca, and K. Folkert Boersma
Atmos. Chem. Phys., 21, 18393–18411, https://doi.org/10.5194/acp-21-18393-2021, https://doi.org/10.5194/acp-21-18393-2021, 2021
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Dry deposition is an important sink for tropospheric ozone that affects ecosystem carbon uptake, but process understanding remains incomplete. We apply a common deposition representation in atmospheric chemistry models and a multi-layer canopy model to multi-year ozone deposition observations. The multi-layer canopy model performs better on diurnal timescales compared to the common approach, leading to a substantially improved simulation of ozone deposition and vegetation ozone impact metrics.
Vilma Kangasaho, Aki Tsuruta, Leif Backman, Pyry Mäkinen, Sander Houweling, Arjo Segers, Maarten Krol, Ed Dlugokencky, Sylvia Michel, James White, and Tuula Aalto
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-843, https://doi.org/10.5194/acp-2021-843, 2021
Revised manuscript not accepted
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Understanding the composition of carbon isotopes can help to better understand the changes in methane budgets. This study investigates how methane sources affect the seasonal cycle of the methane carbon-13 isotope during 2000–2012 using an atmospheric transport model. We found that emissions from both anthropogenic and natural sources contribute. The findings raise a need to revise the magnitudes, proportion, and seasonal cycles of anthropogenic sources and northern wetland emissions.
Maria Sand, Bjørn H. Samset, Gunnar Myhre, Jonas Gliß, Susanne E. Bauer, Huisheng Bian, Mian Chin, Ramiro Checa-Garcia, Paul Ginoux, Zak Kipling, Alf Kirkevåg, Harri Kokkola, Philippe Le Sager, Marianne T. Lund, Hitoshi Matsui, Twan van Noije, Dirk J. L. Olivié, Samuel Remy, Michael Schulz, Philip Stier, Camilla W. Stjern, Toshihiko Takemura, Kostas Tsigaridis, Svetlana G. Tsyro, and Duncan Watson-Parris
Atmos. Chem. Phys., 21, 15929–15947, https://doi.org/10.5194/acp-21-15929-2021, https://doi.org/10.5194/acp-21-15929-2021, 2021
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Absorption of shortwave radiation by aerosols can modify precipitation and clouds but is poorly constrained in models. A total of 15 different aerosol models from AeroCom phase III have reported total aerosol absorption, and for the first time, 11 of these models have reported in a consistent experiment the contributions to absorption from black carbon, dust, and organic aerosol. Here, we document the model diversity in aerosol absorption.
Twan van Noije, Tommi Bergman, Philippe Le Sager, Declan O'Donnell, Risto Makkonen, María Gonçalves-Ageitos, Ralf Döscher, Uwe Fladrich, Jost von Hardenberg, Jukka-Pekka Keskinen, Hannele Korhonen, Anton Laakso, Stelios Myriokefalitakis, Pirkka Ollinaho, Carlos Pérez García-Pando, Thomas Reerink, Roland Schrödner, Klaus Wyser, and Shuting Yang
Geosci. Model Dev., 14, 5637–5668, https://doi.org/10.5194/gmd-14-5637-2021, https://doi.org/10.5194/gmd-14-5637-2021, 2021
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This paper documents the global climate model EC-Earth3-AerChem, one of the members of the EC-Earth3 family of models participating in CMIP6. We give an overview of the model and describe in detail how it differs from its predecessor and the other EC-Earth3 configurations. The model's performance is characterized using coupled simulations conducted for CMIP6. The model has an effective equilibrium climate sensitivity of 3.9 °C and a transient climate response of 2.1 °C.
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.
Ramiro Checa-Garcia, Yves Balkanski, Samuel Albani, Tommi Bergman, Ken Carslaw, Anne Cozic, Chris Dearden, Beatrice Marticorena, Martine Michou, Twan van Noije, Pierre Nabat, Fiona M. O'Connor, Dirk Olivié, Joseph M. Prospero, Philippe Le Sager, Michael Schulz, and Catherine Scott
Atmos. Chem. Phys., 21, 10295–10335, https://doi.org/10.5194/acp-21-10295-2021, https://doi.org/10.5194/acp-21-10295-2021, 2021
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Thousands of tons of dust are emitted into the atmosphere every year, producing important impacts on the Earth system. However, current global climate models are not yet able to reproduce dust emissions, transport and depositions with the desirable accuracy. Our study analyses five different Earth system models to report aspects to be improved to reproduce better available observations, increase the consistency between models and therefore decrease the current uncertainties.
Johannes G. M. Barten, Laurens N. Ganzeveld, Gert-Jan Steeneveld, and Maarten C. Krol
Atmos. Chem. Phys., 21, 10229–10248, https://doi.org/10.5194/acp-21-10229-2021, https://doi.org/10.5194/acp-21-10229-2021, 2021
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We present an evaluation of ocean and snow/ice O3 deposition in explaining observed hourly surface O3 at 25 pan-Arctic sites using an atmospheric meteorology/chemistry model. The model includes a mechanistic representation of ocean O3 deposition as a function of ocean biogeochemical and mixing conditions. The mechanistic representation agrees better with O3 observations in terms of magnitude and temporal variability especially in the High Arctic (> 70° N).
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.
Stijn Naus, Stephen A. Montzka, Prabir K. Patra, and Maarten C. Krol
Atmos. Chem. Phys., 21, 4809–4824, https://doi.org/10.5194/acp-21-4809-2021, https://doi.org/10.5194/acp-21-4809-2021, 2021
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Following up on previous box model studies, we employ a 3D transport model to estimate variations in the hydroxyl radical (OH) from observations of methyl chloroform (MCF). We derive small interannual OH variations that are consistent with variations in the El Niño–Southern Oscillation. We also find evidence for the release of MCF from oceans in atmospheric gradients of MCF. Both findings highlight the added value of a 3D transport model since box model studies did not identify these effects.
Jin Ma, Linda M. J. Kooijmans, Ara Cho, Stephen A. Montzka, Norbert Glatthor, John R. Worden, Le Kuai, Elliot L. Atlas, and Maarten C. Krol
Atmos. Chem. Phys., 21, 3507–3529, https://doi.org/10.5194/acp-21-3507-2021, https://doi.org/10.5194/acp-21-3507-2021, 2021
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Carbonyl sulfide is an important trace gas in the atmosphere and useful to estimating gross primary productivity in ecosystems, but its sources and sinks remain highly uncertain. Therefore, we applied inverse model system TM5-4DVAR to better constrain the global budget. Our finding is in line with earlier studies, pointing to missing sources in the tropics and more uptake in high latitudes. We also stress the necessity of more ground-based observations and satellite data assimilation in future.
Jonas Gliß, Augustin Mortier, Michael Schulz, Elisabeth Andrews, Yves Balkanski, Susanne E. Bauer, Anna M. K. Benedictow, Huisheng Bian, Ramiro Checa-Garcia, Mian Chin, Paul Ginoux, Jan J. Griesfeller, Andreas Heckel, Zak Kipling, Alf Kirkevåg, Harri Kokkola, Paolo Laj, Philippe Le Sager, Marianne Tronstad Lund, Cathrine Lund Myhre, Hitoshi Matsui, Gunnar Myhre, David Neubauer, Twan van Noije, Peter North, Dirk J. L. Olivié, Samuel Rémy, Larisa Sogacheva, Toshihiko Takemura, Kostas Tsigaridis, and Svetlana G. Tsyro
Atmos. Chem. Phys., 21, 87–128, https://doi.org/10.5194/acp-21-87-2021, https://doi.org/10.5194/acp-21-87-2021, 2021
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Simulated aerosol optical properties as well as the aerosol life cycle are investigated for 14 global models participating in the AeroCom initiative. Considerable diversity is found in the simulated aerosol species emissions and lifetimes, also resulting in a large diversity in the simulated aerosol mass, composition, and optical properties. A comparison with observations suggests that, on average, current models underestimate the direct effect of aerosol on the atmosphere radiation budget.
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.
Stelios Myriokefalitakis, Nikos Daskalakis, Angelos Gkouvousis, Andreas Hilboll, Twan van Noije, Jason E. Williams, Philippe Le Sager, Vincent Huijnen, Sander Houweling, Tommi Bergman, Johann Rasmus Nüß, Mihalis Vrekoussis, Maria Kanakidou, and Maarten C. Krol
Geosci. Model Dev., 13, 5507–5548, https://doi.org/10.5194/gmd-13-5507-2020, https://doi.org/10.5194/gmd-13-5507-2020, 2020
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This work documents and evaluates the detailed tropospheric gas-phase chemical mechanism MOGUNTIA in the three-dimensional chemistry transport model TM5-MP. The Rosenbrock solver, as generated by the KPP software, is implemented in the chemistry code, which can successfully replace the classical Euler backward integration method. The MOGUNTIA scheme satisfactorily simulates a large suite of oxygenated volatile organic compounds (VOCs) that are observed in the atmosphere at significant levels.
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.
Srijana Lama, Sander Houweling, K. Folkert Boersma, Henk Eskes, Ilse Aben, Hugo A. C. Denier van der Gon, Maarten C. Krol, Han Dolman, Tobias Borsdorff, and Alba Lorente
Atmos. Chem. Phys., 20, 10295–10310, https://doi.org/10.5194/acp-20-10295-2020, https://doi.org/10.5194/acp-20-10295-2020, 2020
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Rapid urbanization has increased the consumption of fossil fuel, contributing the degradation of urban air quality. Burning efficiency is a major factor determining the impact of fuel burning on the environment. We quantify the burning efficiency of fossil fuel use over six megacities using satellite remote sensing data. City governance can use these results to understand air pollution scenarios and to formulate effective air pollution control strategies.
María A. Burgos, Elisabeth Andrews, Gloria Titos, Angela Benedetti, Huisheng Bian, Virginie Buchard, Gabriele Curci, Zak Kipling, Alf Kirkevåg, Harri Kokkola, Anton Laakso, Julie Letertre-Danczak, Marianne T. Lund, Hitoshi Matsui, Gunnar Myhre, Cynthia Randles, Michael Schulz, Twan van Noije, Kai Zhang, Lucas Alados-Arboledas, Urs Baltensperger, Anne Jefferson, James Sherman, Junying Sun, Ernest Weingartner, and Paul Zieger
Atmos. Chem. Phys., 20, 10231–10258, https://doi.org/10.5194/acp-20-10231-2020, https://doi.org/10.5194/acp-20-10231-2020, 2020
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We investigate how well models represent the enhancement in scattering coefficients due to particle water uptake, and perform an evaluation of several implementation schemes used in ten Earth system models. Our results show the importance of the parameterization of hygroscopicity and model chemistry as drivers of some of the observed diversity amongst model estimates. The definition of dry conditions and the phenomena taking place in this relative humidity range also impact the model evaluation.
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.
Robert J. Allen, Steven Turnock, Pierre Nabat, David Neubauer, Ulrike Lohmann, Dirk Olivié, Naga Oshima, Martine Michou, Tongwen Wu, Jie Zhang, Toshihiko Takemura, Michael Schulz, Kostas Tsigaridis, Susanne E. Bauer, Louisa Emmons, Larry Horowitz, Vaishali Naik, Twan van Noije, Tommi Bergman, Jean-Francois Lamarque, Prodromos Zanis, Ina Tegen, Daniel M. Westervelt, Philippe Le Sager, Peter Good, Sungbo Shim, Fiona O'Connor, Dimitris Akritidis, Aristeidis K. Georgoulias, Makoto Deushi, Lori T. Sentman, Jasmin G. John, Shinichiro Fujimori, and William J. Collins
Atmos. Chem. Phys., 20, 9641–9663, https://doi.org/10.5194/acp-20-9641-2020, https://doi.org/10.5194/acp-20-9641-2020, 2020
Johannes G. M. Barten, Laurens N. Ganzeveld, Auke J. Visser, Rodrigo Jiménez, and Maarten C. Krol
Atmos. Chem. Phys., 20, 9441–9458, https://doi.org/10.5194/acp-20-9441-2020, https://doi.org/10.5194/acp-20-9441-2020, 2020
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Combining satellite and urban air pollution measurements with a meteorology and air quality model, we present the state of air quality in Colombia. We found four distinctly different emission regimes. The simulated pollution levels compare well with satellite data, but the comparison also indicates misrepresentation of prescribed fire emissions and simulated lightning emissions. Comparison of urban measurements requires careful consideration of (nocturnal) boundary layer dynamics and advection.
Rein Haarsma, Mario Acosta, Rena Bakhshi, Pierre-Antoine Bretonnière, Louis-Philippe Caron, Miguel Castrillo, Susanna Corti, Paolo Davini, Eleftheria Exarchou, Federico Fabiano, Uwe Fladrich, Ramon Fuentes Franco, Javier García-Serrano, Jost von Hardenberg, Torben Koenigk, Xavier Levine, Virna Loana Meccia, Twan van Noije, Gijs van den Oord, Froila M. Palmeiro, Mario Rodrigo, Yohan Ruprich-Robert, Philippe Le Sager, Etienne Tourigny, Shiyu Wang, Michiel van Weele, and Klaus Wyser
Geosci. Model Dev., 13, 3507–3527, https://doi.org/10.5194/gmd-13-3507-2020, https://doi.org/10.5194/gmd-13-3507-2020, 2020
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HighResMIP is an international coordinated CMIP6 effort to investigate the improvement in climate modeling caused by an increase in horizontal resolution. This paper describes EC-Earth3P-(HR), which has been developed for HighResMIP. First analyses reveal that increasing resolution does improve certain aspects of the simulated climate but that many other biases still continue, possibly related to phenomena that are still not yet resolved and need to be parameterized.
Klaus Wyser, Twan van Noije, Shuting Yang, Jost von Hardenberg, Declan O'Donnell, and Ralf Döscher
Geosci. Model Dev., 13, 3465–3474, https://doi.org/10.5194/gmd-13-3465-2020, https://doi.org/10.5194/gmd-13-3465-2020, 2020
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The EC-Earth model used for CMIP6 is found to have a higher equilibrium climate sensitivity (ECS) than its predecessor used for CMIP5. In a series of sensitivity experiments, we investigate which model updates since CMIP5 have contributed to the increase in ECS. The main reason for the higher sensitivity in the EC-Earth model is the improved representation of the aerosol–radiation and aerosol–cloud interactions.
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).
Moa K. Sporre, Sara M. Blichner, Roland Schrödner, Inger H. H. Karset, Terje K. Berntsen, Twan van Noije, Tommi Bergman, Declan O'Donnell, and Risto Makkonen
Atmos. Chem. Phys., 20, 8953–8973, https://doi.org/10.5194/acp-20-8953-2020, https://doi.org/10.5194/acp-20-8953-2020, 2020
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We investigate how emissions and parameters in current
SOA parameterisations in three ESMs affect both the resulting SOA in the models and the impact this has on climate through the direct and indirect aerosol effects. The SOA changes induce very different responses in the models, especially in terms of the indirect aerosol effect. This introduces uncertainties in ESM estimates of SOA climate impact through feedbacks in a warming climate and through anthropogenic land use change.
Marielle Saunois, Ann R. Stavert, Ben Poulter, Philippe Bousquet, Josep G. Canadell, Robert B. Jackson, Peter A. Raymond, Edward J. Dlugokencky, Sander Houweling, Prabir K. Patra, Philippe Ciais, Vivek K. Arora, David Bastviken, Peter Bergamaschi, Donald R. Blake, Gordon Brailsford, Lori Bruhwiler, Kimberly M. Carlson, Mark Carrol, Simona Castaldi, Naveen Chandra, Cyril Crevoisier, Patrick M. Crill, Kristofer Covey, Charles L. Curry, Giuseppe Etiope, Christian Frankenberg, Nicola Gedney, Michaela I. Hegglin, Lena Höglund-Isaksson, Gustaf Hugelius, Misa Ishizawa, Akihiko Ito, Greet Janssens-Maenhout, Katherine M. Jensen, Fortunat Joos, Thomas Kleinen, Paul B. Krummel, Ray L. Langenfelds, Goulven G. Laruelle, Licheng Liu, Toshinobu Machida, Shamil Maksyutov, Kyle C. McDonald, Joe McNorton, Paul A. Miller, Joe R. Melton, Isamu Morino, Jurek Müller, Fabiola Murguia-Flores, Vaishali Naik, Yosuke Niwa, Sergio Noce, Simon O'Doherty, Robert J. Parker, Changhui Peng, Shushi Peng, Glen P. Peters, Catherine Prigent, Ronald Prinn, Michel Ramonet, Pierre Regnier, William J. Riley, Judith A. Rosentreter, Arjo Segers, Isobel J. Simpson, Hao Shi, Steven J. Smith, L. Paul Steele, Brett F. Thornton, Hanqin Tian, Yasunori Tohjima, Francesco N. Tubiello, Aki Tsuruta, Nicolas Viovy, Apostolos Voulgarakis, Thomas S. Weber, Michiel van Weele, Guido R. van der Werf, Ray F. Weiss, Doug Worthy, Debra Wunch, Yi Yin, Yukio Yoshida, Wenxin Zhang, Zhen Zhang, Yuanhong Zhao, Bo Zheng, Qing Zhu, Qiuan Zhu, and Qianlai Zhuang
Earth Syst. Sci. Data, 12, 1561–1623, https://doi.org/10.5194/essd-12-1561-2020, https://doi.org/10.5194/essd-12-1561-2020, 2020
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Understanding and quantifying the global methane (CH4) budget is important for assessing realistic pathways to mitigate climate change. We have established a consortium of multidisciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate new research aimed at improving and regularly updating the global methane budget. This is the second version of the review dedicated to the decadal methane budget, integrating results of top-down and bottom-up estimates.
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.
Auke J. Visser, K. Folkert Boersma, Laurens N. Ganzeveld, and Maarten C. Krol
Atmos. Chem. Phys., 19, 11821–11841, https://doi.org/10.5194/acp-19-11821-2019, https://doi.org/10.5194/acp-19-11821-2019, 2019
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Health and ecosystem impacts of O3 generally occur when O3 concentrations are highest, but most air quality models underestimate peak O3. We derived European NOx emissions based on satellite NO2 column data and evaluated the impact on model-simulated NO2 and ozone. We show that a simulation with satellite-derived NOx emissions leads to better agreement with independent in situ observations of surface NO2 and O3, which helps to reduce the model underestimations of peak ozone concentrations.
George S. Fanourgakis, Maria Kanakidou, Athanasios Nenes, Susanne E. Bauer, Tommi Bergman, Ken S. Carslaw, Alf Grini, Douglas S. Hamilton, Jill S. Johnson, Vlassis A. Karydis, Alf Kirkevåg, John K. Kodros, Ulrike Lohmann, Gan Luo, Risto Makkonen, Hitoshi Matsui, David Neubauer, Jeffrey R. Pierce, Julia Schmale, Philip Stier, Kostas Tsigaridis, Twan van Noije, Hailong Wang, Duncan Watson-Parris, Daniel M. Westervelt, Yang Yang, Masaru Yoshioka, Nikos Daskalakis, Stefano Decesari, Martin Gysel-Beer, Nikos Kalivitis, Xiaohong Liu, Natalie M. Mahowald, Stelios Myriokefalitakis, Roland Schrödner, Maria Sfakianaki, Alexandra P. Tsimpidi, Mingxuan Wu, and Fangqun Yu
Atmos. Chem. Phys., 19, 8591–8617, https://doi.org/10.5194/acp-19-8591-2019, https://doi.org/10.5194/acp-19-8591-2019, 2019
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Effects of aerosols on clouds are important for climate studies but are among the largest uncertainties in climate projections. This study evaluates the skill of global models to simulate aerosol, cloud condensation nuclei (CCN) and cloud droplet number concentrations (CDNCs). Model results show reduced spread in CDNC compared to CCN due to the negative correlation between the sensitivities of CDNC to aerosol number concentration (air pollution) and updraft velocity (atmospheric dynamics).
Stephanie Fiedler, Stefan Kinne, Wan Ting Katty Huang, Petri Räisänen, Declan O'Donnell, Nicolas Bellouin, Philip Stier, Joonas Merikanto, Twan van Noije, Risto Makkonen, and Ulrike Lohmann
Atmos. Chem. Phys., 19, 6821–6841, https://doi.org/10.5194/acp-19-6821-2019, https://doi.org/10.5194/acp-19-6821-2019, 2019
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
Juhi Nagori, Ruud H. H. Janssen, Juliane L. Fry, Maarten Krol, Jose L. Jimenez, Weiwei Hu, and Jordi Vilà-Guerau de Arellano
Atmos. Chem. Phys., 19, 701–729, https://doi.org/10.5194/acp-19-701-2019, https://doi.org/10.5194/acp-19-701-2019, 2019
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Secondary organic aerosol (SOA) is produced through a complex interaction of sunlight, volatile organic compounds emitted from trees, anthropogenic emissions, and atmospheric chemistry. We are able to successfully model the formation and diurnal evolution of SOA using a model that takes into consideration the surface and boundary layer dynamics (1–2 km from the surface) and photochemistry above the southeastern US with data collected during the SOAS campaign to constrain the model.
Stijn Naus, Stephen A. Montzka, Sudhanshu Pandey, Sourish Basu, Ed J. Dlugokencky, and Maarten Krol
Atmos. Chem. Phys., 19, 407–424, https://doi.org/10.5194/acp-19-407-2019, https://doi.org/10.5194/acp-19-407-2019, 2019
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We investigate how the use of a two-box model to describe the troposphere can impact derived results, relative to more complex models. For this, we use a 3-D transport model to tune a two-box model of OH, CH4, and MCF. By comparing the tuned two-box model with a standard model run, we can diagnose and quantify biases inherent to a two-box model. We find strong biases, but these have only a small impact on our final conclusions. However, it is not obvious that this should hold for future studies.
Stelios Myriokefalitakis, Akinori Ito, Maria Kanakidou, Athanasios Nenes, Maarten C. Krol, Natalie M. Mahowald, Rachel A. Scanza, Douglas S. Hamilton, Matthew S. Johnson, Nicholas Meskhidze, Jasper F. Kok, Cecile Guieu, Alex R. Baker, Timothy D. Jickells, Manmohan M. Sarin, Srinivas Bikkina, Rachel Shelley, Andrew Bowie, Morgane M. G. Perron, and Robert A. Duce
Biogeosciences, 15, 6659–6684, https://doi.org/10.5194/bg-15-6659-2018, https://doi.org/10.5194/bg-15-6659-2018, 2018
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The first atmospheric iron (Fe) deposition model intercomparison is presented in this study, as a result of the deliberations of the United Nations Joint Group of Experts on the Scientific Aspects of Marine Environmental Protection (GESAMP; http://www.gesamp.org/) Working Group 38. We conclude that model diversity over remote oceans reflects uncertainty in the Fe content parameterizations of dust aerosols, combustion aerosol emissions and the size distribution of transported aerosol Fe.
Maarten Krol, Marco de Bruine, Lars Killaars, Huug Ouwersloot, Andrea Pozzer, Yi Yin, Frederic Chevallier, Philippe Bousquet, Prabir Patra, Dmitry Belikov, Shamil Maksyutov, Sandip Dhomse, Wuhu Feng, and Martyn P. Chipperfield
Geosci. Model Dev., 11, 3109–3130, https://doi.org/10.5194/gmd-11-3109-2018, https://doi.org/10.5194/gmd-11-3109-2018, 2018
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The TransCom inter-comparison project regularly carries out studies to quantify errors in simulated atmospheric transport. This paper presents the first results of an age of air (AoA) inter-comparison of six global transport models. Following a protocol, six models simulated five tracers from which atmospheric transport times can easily be deduced. Results highlight that inter-model differences associated with atmospheric transport are still large and require further analysis.
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.
Geert Jan van Oldenborgh, Sjoukje Philip, Sarah Kew, Michiel van Weele, Peter Uhe, Friederike Otto, Roop Singh, Indrani Pai, Heidi Cullen, and Krishna AchutaRao
Nat. Hazards Earth Syst. Sci., 18, 365–381, https://doi.org/10.5194/nhess-18-365-2018, https://doi.org/10.5194/nhess-18-365-2018, 2018
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On 19 May 2016 a temperature of 51.0 °C in Phalodi (northwest India) set a new Indian record. In 2015 a very lethal heat wave had occurred in the southeast. We find that in India the trend in extreme temperatures due to greenhouse gases is largely cancelled by increasing air pollution and irrigation. The health impacts of heat waves do increase due to higher humidity and air pollution. This implies that we expect heat waves to become much hotter as soon as air pollution is brought under control.
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.
Maria Sand, Bjørn H. Samset, Yves Balkanski, Susanne Bauer, Nicolas Bellouin, Terje K. Berntsen, Huisheng Bian, Mian Chin, Thomas Diehl, Richard Easter, Steven J. Ghan, Trond Iversen, Alf Kirkevåg, Jean-François Lamarque, Guangxing Lin, Xiaohong Liu, Gan Luo, Gunnar Myhre, Twan van Noije, Joyce E. Penner, Michael Schulz, Øyvind Seland, Ragnhild B. Skeie, Philip Stier, Toshihiko Takemura, Kostas Tsigaridis, Fangqun Yu, Kai Zhang, and Hua Zhang
Atmos. Chem. Phys., 17, 12197–12218, https://doi.org/10.5194/acp-17-12197-2017, https://doi.org/10.5194/acp-17-12197-2017, 2017
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The role of aerosols in the changing polar climate is not well understood and the aerosols are poorly constrained in the models. In this study we have compared output from 16 different aerosol models with available observations at both poles. We show that the model median is representative of the observations, but the model spread is large. The Arctic direct aerosol radiative effect over the industrial area is positive during spring due to black carbon and negative during summer due to sulfate.
Ingrid T. van der Laan-Luijkx, Ivar R. van der Velde, Emma van der Veen, Aki Tsuruta, Karolina Stanislawska, Arne Babenhauserheide, Hui Fang Zhang, Yu Liu, Wei He, Huilin Chen, Kenneth A. Masarie, Maarten C. Krol, and Wouter Peters
Geosci. Model Dev., 10, 2785–2800, https://doi.org/10.5194/gmd-10-2785-2017, https://doi.org/10.5194/gmd-10-2785-2017, 2017
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The CarbonTracker Data Assimilation Shell (CTDAS) is the new modular implementation of the CarbonTracker Europe (CTE) data assimilation system. We present and document CTDAS and demonstrate its ability to estimate global carbon sources and sinks. We present the latest CTE results including the distribution of the carbon sinks over the hemispheres and between the land biosphere and the oceans. We show the versatility of CTDAS with an overview of the wide range of other applications.
Melina-Maria Zempila, Jos H. G. M. van Geffen, Michael Taylor, Ilias Fountoulakis, Maria-Elissavet Koukouli, Michiel van Weele, Ronald J. van der A, Alkiviadis Bais, Charikleia Meleti, and Dimitrios Balis
Atmos. Chem. Phys., 17, 7157–7174, https://doi.org/10.5194/acp-17-7157-2017, https://doi.org/10.5194/acp-17-7157-2017, 2017
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NILU irradiances at five UV channels were used to produce CIE, vitamin D, and DNA- damage daily doses via a neural network (NN) model. The NN was trained with collocated weighted Brewer spectra and uncertainty in the NILU-derived UV effective doses was 7.5 %. TEMIS UV products were found to be ~ 12.5 % higher than the NILU estimates. The results improve for cloud-free days with differences of 0.57 % for CIE, 1.22 % for vitamin D, and 1.18 % for DNA damage, with standard deviations of ~ 11–13 %.
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.
Aki Tsuruta, Tuula Aalto, Leif Backman, Janne Hakkarainen, Ingrid T. van der Laan-Luijkx, Maarten C. Krol, Renato Spahni, Sander Houweling, Marko Laine, Ed Dlugokencky, Angel J. Gomez-Pelaez, Marcel van der Schoot, Ray Langenfelds, Raymond Ellul, Jgor Arduini, Francesco Apadula, Christoph Gerbig, Dietrich G. Feist, Rigel Kivi, Yukio Yoshida, and Wouter Peters
Geosci. Model Dev., 10, 1261–1289, https://doi.org/10.5194/gmd-10-1261-2017, https://doi.org/10.5194/gmd-10-1261-2017, 2017
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In this study, we found that the average global methane emission for 2000–2012, estimated by the CTE-CH4 model, was 516±51 Tg CH4 yr-1, and the estimates for 2007–2012 were 4 % larger than for 2000–2006. The model estimates are sensitive to inputs and setups, but according to sensitivity tests the study suggests that the increase in atmospheric methane concentrations during 21st century was due to an increase in emissions from the 35S-EQ latitudinal bands.
Alba Lorente, K. Folkert Boersma, Huan Yu, Steffen Dörner, Andreas Hilboll, Andreas Richter, Mengyao Liu, Lok N. Lamsal, Michael Barkley, Isabelle De Smedt, Michel Van Roozendael, Yang Wang, Thomas Wagner, Steffen Beirle, Jin-Tai Lin, Nickolay Krotkov, Piet Stammes, Ping Wang, Henk J. Eskes, and Maarten Krol
Atmos. Meas. Tech., 10, 759–782, https://doi.org/10.5194/amt-10-759-2017, https://doi.org/10.5194/amt-10-759-2017, 2017
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Choices and assumptions made to represent the state of the atmosphere introduce an uncertainty of 42 % in the air mass factor calculation in trace gas satellite retrievals in polluted regions. The AMF strongly depends on the choice of a priori trace gas profile, surface albedo data set and the correction method to account for clouds and aerosols. We call for well-designed validation exercises focusing on situations when AMF structural uncertainty has the highest impact on satellite retrievals.
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.
Sander Houweling, Peter Bergamaschi, Frederic Chevallier, Martin Heimann, Thomas Kaminski, Maarten Krol, Anna M. Michalak, and Prabir Patra
Atmos. Chem. Phys., 17, 235–256, https://doi.org/10.5194/acp-17-235-2017, https://doi.org/10.5194/acp-17-235-2017, 2017
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The aim of this paper is to present an overview of inverse modeling methods, developed over the years, for estimating the global sources and sinks of the greenhouse gas methane from atmospheric measurements. It provides insight into how techniques and estimates have evolved over time, what the remaining shortcomings are, new developments, and promising future directions.
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
Marielle Saunois, Philippe Bousquet, Ben Poulter, Anna Peregon, Philippe Ciais, Josep G. Canadell, Edward J. Dlugokencky, Giuseppe Etiope, David Bastviken, Sander Houweling, Greet Janssens-Maenhout, Francesco N. Tubiello, Simona Castaldi, Robert B. Jackson, Mihai Alexe, Vivek K. Arora, David J. Beerling, Peter Bergamaschi, Donald R. Blake, Gordon Brailsford, Victor Brovkin, Lori Bruhwiler, Cyril Crevoisier, Patrick Crill, Kristofer Covey, Charles Curry, Christian Frankenberg, Nicola Gedney, Lena Höglund-Isaksson, Misa Ishizawa, Akihiko Ito, Fortunat Joos, Heon-Sook Kim, Thomas Kleinen, Paul Krummel, Jean-François Lamarque, Ray Langenfelds, Robin Locatelli, Toshinobu Machida, Shamil Maksyutov, Kyle C. McDonald, Julia Marshall, Joe R. Melton, Isamu Morino, Vaishali Naik, Simon O'Doherty, Frans-Jan W. Parmentier, Prabir K. Patra, Changhui Peng, Shushi Peng, Glen P. Peters, Isabelle Pison, Catherine Prigent, Ronald Prinn, Michel Ramonet, William J. Riley, Makoto Saito, Monia Santini, Ronny Schroeder, Isobel J. Simpson, Renato Spahni, Paul Steele, Atsushi Takizawa, Brett F. Thornton, Hanqin Tian, Yasunori Tohjima, Nicolas Viovy, Apostolos Voulgarakis, Michiel van Weele, Guido R. van der Werf, Ray Weiss, Christine Wiedinmyer, David J. Wilton, Andy Wiltshire, Doug Worthy, Debra Wunch, Xiyan Xu, Yukio Yoshida, Bowen Zhang, Zhen Zhang, and Qiuan Zhu
Earth Syst. Sci. Data, 8, 697–751, https://doi.org/10.5194/essd-8-697-2016, https://doi.org/10.5194/essd-8-697-2016, 2016
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An accurate assessment of the methane budget is important to understand the atmospheric methane concentrations and trends and to provide realistic pathways for climate change mitigation. The various and diffuse sources of methane as well and its oxidation by a very short lifetime radical challenge this assessment. We quantify the methane sources and sinks as well as their uncertainties based on both bottom-up and top-down approaches provided by a broad international scientific community.
Quentin Errera, Simone Ceccherini, Yves Christophe, Simon Chabrillat, Michaela I. Hegglin, Alyn Lambert, Richard Ménard, Piera Raspollini, Sergey Skachko, Michiel van Weele, and Kaley A. Walker
Atmos. Meas. Tech., 9, 5895–5909, https://doi.org/10.5194/amt-9-5895-2016, https://doi.org/10.5194/amt-9-5895-2016, 2016
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When this study started, its goal was to provide a reanalysis of the stratospheric composition of methane and nitrous oxide, two important sources of hydrogen and nitrogen species in the stratosphere that influence the ozone abundance. However, the goal changed when several issues in the assimilated observations were discovered. Finally, this study illustrates how data assimilation methods can be used to add value to the observations as well as to diagnose their limitations.
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.
E. N. Koffi, P. Bergamaschi, U. Karstens, M. Krol, A. Segers, M. Schmidt, I. Levin, A. T. Vermeulen, R. E. Fisher, V. Kazan, H. Klein Baltink, D. Lowry, G. Manca, H. A. J. Meijer, J. Moncrieff, S. Pal, M. Ramonet, H. A. Scheeren, and A. G. Williams
Geosci. Model Dev., 9, 3137–3160, https://doi.org/10.5194/gmd-9-3137-2016, https://doi.org/10.5194/gmd-9-3137-2016, 2016
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We evaluate the capability of the TM5 model to reproduce observations of the boundary layer dynamics and the associated variability of trace gases close to the surface, using 222Rn. Focusing on the European scale, we compare the TM5 boundary layer heights with observations from radiosondes, lidar, and ceilometer. Furthermore, we compare TM5 simulations of 222Rn activity concentrations, using a novel, process-based 222Rn flux map over Europe, with 222Rn harmonized measurements from 10 stations.
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.
Aki Tsuruta, Tuula Aalto, Leif Backman, Janne Hakkarainen, Ingrid T. van der Laan-Luijkx, Maarten C. Krol, Renato Spahni, Sander Houweling, Marko Laine, Marcel van der Schoot, Ray Langenfelds, Raymond Ellul, and Wouter Peters
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2016-181, https://doi.org/10.5194/gmd-2016-181, 2016
Revised manuscript has not been submitted
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In this study, we found that methane emission estimates, driven by the CTE-CH4 model, depend on model setups and inputs, especially for regional estimates. An optimal setup makes the estimates stable, but inputs, such as emission estimates from inventories, and observations, also play significant role. The results can be used for an extended analysis on relative contributions of methane emissions to atmospheric methane concentration changes in recent decades.
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.
Chul E. Chung, Jung-Eun Chu, Yunha Lee, Twan van Noije, Hwayoung Jeoung, Kyung-Ja Ha, and Marguerite Marks
Atmos. Chem. Phys., 16, 8071–8080, https://doi.org/10.5194/acp-16-8071-2016, https://doi.org/10.5194/acp-16-8071-2016, 2016
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Currently, the magnitude of aerosol direct forcing is estimated to range from −0.85 W m−2 to +0.15 W m−2. The uncertainty in estimated aerosol direct forcing is largely due to uncertainties in global aerosol simulation models. We processed a comprehensive suite of observations and developed creative uses of observations to constrain aerosol simulations. The net results are that (i) we reduced the forcing uncertainty and (ii) we showed that the forcing must be less negative than the consensus.
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.
Zak Kipling, Philip Stier, Colin E. Johnson, Graham W. Mann, Nicolas Bellouin, Susanne E. Bauer, Tommi Bergman, Mian Chin, Thomas Diehl, Steven J. Ghan, Trond Iversen, Alf Kirkevåg, Harri Kokkola, Xiaohong Liu, Gan Luo, Twan van Noije, Kirsty J. Pringle, Knut von Salzen, Michael Schulz, Øyvind Seland, Ragnhild B. Skeie, Toshihiko Takemura, Kostas Tsigaridis, and Kai Zhang
Atmos. Chem. Phys., 16, 2221–2241, https://doi.org/10.5194/acp-16-2221-2016, https://doi.org/10.5194/acp-16-2221-2016, 2016
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The vertical distribution of atmospheric aerosol is an important factor in its effects on climate. In this study we use a sophisticated model of the many interacting processes affecting aerosol in the atmosphere to show that the vertical distribution is typically dominated by only a few of these processes. Constraining these physical processes may help to reduce the large differences between models. However, the important processes are not always the same for different types of aerosol.
M. K. van der Molen, R. A. M. de Jeu, W. Wagner, I. R. van der Velde, P. Kolari, J. Kurbatova, A. Varlagin, T. C. Maximov, A. V. Kononov, T. Ohta, A. Kotani, M. C. Krol, and W. Peters
Hydrol. Earth Syst. Sci., 20, 605–624, https://doi.org/10.5194/hess-20-605-2016, https://doi.org/10.5194/hess-20-605-2016, 2016
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Boreal Eurasia contains extensive forests, which play an important role in the terrestrial carbon cycle. Droughts can modify this cycle considerably, although very few ground-based observations are available in the region. We test whether satellite-observed soil moisture may be used to improve carbon cycle models in this region. This paper explains when and where this works best. The interpretation of satellite soil moisture is best in summer conditions, and is hampered by snow, ice and ponding.
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.
I. R. van der Velde, J. B. Miller, K. Schaefer, G. R. van der Werf, M. C. Krol, and W. Peters
Biogeosciences, 11, 6553–6571, https://doi.org/10.5194/bg-11-6553-2014, https://doi.org/10.5194/bg-11-6553-2014, 2014
T. P. C. van Noije, P. Le Sager, A. J. Segers, P. F. J. van Velthoven, M. C. Krol, W. Hazeleger, A. G. Williams, and S. D. Chambers
Geosci. Model Dev., 7, 2435–2475, https://doi.org/10.5194/gmd-7-2435-2014, https://doi.org/10.5194/gmd-7-2435-2014, 2014
K. Tsigaridis, N. Daskalakis, M. Kanakidou, P. J. Adams, P. Artaxo, R. Bahadur, Y. Balkanski, S. E. Bauer, N. Bellouin, A. Benedetti, T. Bergman, T. K. Berntsen, J. P. Beukes, H. Bian, K. S. Carslaw, M. Chin, G. Curci, T. Diehl, R. C. Easter, S. J. Ghan, S. L. Gong, A. Hodzic, C. R. Hoyle, T. Iversen, S. Jathar, J. L. Jimenez, J. W. Kaiser, A. Kirkevåg, D. Koch, H. Kokkola, Y. H Lee, G. Lin, X. Liu, G. Luo, X. Ma, G. W. Mann, N. Mihalopoulos, J.-J. Morcrette, J.-F. Müller, G. Myhre, S. Myriokefalitakis, N. L. Ng, D. O'Donnell, J. E. Penner, L. Pozzoli, K. J. Pringle, L. M. Russell, M. Schulz, J. Sciare, Ø. Seland, D. T. Shindell, S. Sillman, R. B. Skeie, D. Spracklen, T. Stavrakou, S. D. Steenrod, T. Takemura, P. Tiitta, S. Tilmes, H. Tost, T. van Noije, P. G. van Zyl, K. von Salzen, F. Yu, Z. Wang, Z. Wang, R. A. Zaveri, H. Zhang, K. Zhang, Q. Zhang, and X. Zhang
Atmos. Chem. Phys., 14, 10845–10895, https://doi.org/10.5194/acp-14-10845-2014, https://doi.org/10.5194/acp-14-10845-2014, 2014
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
D. Bozhinova, M. K. van der Molen, I. R. van der Velde, M. C. Krol, S. van der Laan, H. A. J. Meijer, and W. Peters
Atmos. Chem. Phys., 14, 7273–7290, https://doi.org/10.5194/acp-14-7273-2014, https://doi.org/10.5194/acp-14-7273-2014, 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
P. N. Foster, I. C. Prentice, C. Morfopoulos, M. Siddall, and M. van Weele
Biogeosciences, 11, 3437–3451, https://doi.org/10.5194/bg-11-3437-2014, https://doi.org/10.5194/bg-11-3437-2014, 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
G. W. Mann, K. S. Carslaw, C. L. Reddington, K. J. Pringle, M. Schulz, A. Asmi, D. V. Spracklen, D. A. Ridley, M. T. Woodhouse, L. A. Lee, K. Zhang, S. J. Ghan, R. C. Easter, X. Liu, P. Stier, Y. H. Lee, P. J. Adams, H. Tost, J. Lelieveld, S. E. Bauer, K. Tsigaridis, T. P. C. van Noije, A. Strunk, E. Vignati, N. Bellouin, M. Dalvi, C. E. Johnson, T. Bergman, H. Kokkola, K. von Salzen, F. Yu, G. Luo, A. Petzold, J. Heintzenberg, A. Clarke, J. A. Ogren, J. Gras, U. Baltensperger, U. Kaminski, S. G. Jennings, C. D. O'Dowd, R. M. Harrison, D. C. S. Beddows, M. Kulmala, Y. Viisanen, V. Ulevicius, N. Mihalopoulos, V. Zdimal, M. Fiebig, H.-C. Hansson, E. Swietlicki, and J. S. Henzing
Atmos. Chem. Phys., 14, 4679–4713, https://doi.org/10.5194/acp-14-4679-2014, https://doi.org/10.5194/acp-14-4679-2014, 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
C. Jiao, M. G. Flanner, Y. Balkanski, S. E. Bauer, N. Bellouin, T. K. Berntsen, H. Bian, K. S. Carslaw, M. Chin, N. De Luca, T. Diehl, S. J. Ghan, T. Iversen, A. Kirkevåg, D. Koch, X. Liu, G. W. Mann, J. E. Penner, G. Pitari, M. Schulz, Ø. Seland, R. B. Skeie, S. D. Steenrod, P. Stier, T. Takemura, K. Tsigaridis, T. van Noije, Y. Yun, and K. Zhang
Atmos. Chem. Phys., 14, 2399–2417, https://doi.org/10.5194/acp-14-2399-2014, https://doi.org/10.5194/acp-14-2399-2014, 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
R. Locatelli, P. Bousquet, F. Chevallier, A. Fortems-Cheney, S. Szopa, M. Saunois, A. Agusti-Panareda, D. Bergmann, H. Bian, P. Cameron-Smith, M. P. Chipperfield, E. Gloor, S. Houweling, S. R. Kawa, M. Krol, P. K. Patra, R. G. Prinn, M. Rigby, R. Saito, and C. Wilson
Atmos. Chem. Phys., 13, 9917–9937, https://doi.org/10.5194/acp-13-9917-2013, https://doi.org/10.5194/acp-13-9917-2013, 2013
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
V. Naik, A. Voulgarakis, A. M. Fiore, L. W. Horowitz, J.-F. Lamarque, M. Lin, M. J. Prather, P. J. Young, D. Bergmann, P. J. Cameron-Smith, I. Cionni, W. J. Collins, S. B. Dalsøren, R. Doherty, V. Eyring, G. Faluvegi, G. A. Folberth, B. Josse, Y. H. Lee, I. A. MacKenzie, T. Nagashima, T. P. C. van Noije, D. A. Plummer, M. Righi, S. T. Rumbold, R. Skeie, D. T. Shindell, D. S. Stevenson, S. Strode, K. Sudo, S. Szopa, and G. Zeng
Atmos. Chem. Phys., 13, 5277–5298, https://doi.org/10.5194/acp-13-5277-2013, https://doi.org/10.5194/acp-13-5277-2013, 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
M. Krol, W. Peters, P. Hooghiemstra, M. George, C. Clerbaux, D. Hurtmans, D. McInerney, F. Sedano, P. Bergamaschi, M. El Hajj, J. W. Kaiser, D. Fisher, V. Yershov, and J.-P. Muller
Atmos. Chem. Phys., 13, 4737–4747, https://doi.org/10.5194/acp-13-4737-2013, https://doi.org/10.5194/acp-13-4737-2013, 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
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Sensitivity of climate effects of hydrogen to leakage size, location, and chemical background
Evaluating tropospheric nitrogen dioxide in UKCA using OMI satellite retrievals over south and east Asia
Technical note: A comparative study of chemistry schemes for volcanic sulfur dioxide in Lagrangian transport simulations – a case study of the 2019 Raikoke eruption
Revisiting the high tropospheric ozone over southern Africa: role of biomass burning and anthropogenic emissions
Monoterpene oxidation pathways initiated by acyl peroxy radical addition
Local and transboundary contributions to NOy loadings across East Asia using CMAQ-ISAM and a GEMS-informed emission inventory during the winter–spring transition
Estimating the variability in NOx emissions from Wuhan with TROPOMI NO2 data during 2018 to 2023
Enhanced understanding of atmospheric blocking modulation on ozone dynamics within a high-resolution Earth system model
Natural emissions of VOC and NOx over Africa constrained by TROPOMI HCHO and NO2 data using the MAGRITTEv1.1 model
Anthropogenic emission controls reduce summertime ozone–temperature sensitivity in the United States
Investigating the response of China's surface ozone concentration to the future changes of multiple factors
Assessing the relative impacts of satellite ozone and its precursor observations to improve global tropospheric ozone analysis using multiple chemical reanalysis systems
Evaluating present-day and future impacts of agricultural ammonia emissions on atmospheric chemistry and climate
Air-pollution-satellite-based CO2 emission inversion: system evaluation, sensitivity analysis, and future research direction
Insights into ozone pollution control in urban areas by decoupling meteorological factors based on machine learning
Quantification of regional net CO2 flux errors in the Orbiting Carbon Observatory-2 (OCO-2) v10 model intercomparison project (MIP) ensemble using airborne measurements
Reactive nitrogen in and around the northeastern and mid-Atlantic US: sources, sinks, and connections with ozone
Preindustrial-to-present-day changes in atmospheric carbon monoxide: agreement and gaps between ice archives and global model reconstructions
Investigating processes influencing simulation of local Arctic wintertime anthropogenic pollution in Fairbanks, Alaska, during ALPACA-2022
Urban ozone formation and sensitivities to volatile chemical products, cooking emissions, and NOx upwind of and within two Los Angeles Basin cities
Causes of growing middle-to-upper tropospheric ozone over the northwest Pacific region
Impact of introducing electric vehicles on ground-level O3 and PM2.5 in the Greater Tokyo Area: yearly trends and the importance of changes in the urban heat island effect
Modelling Arctic Lower Tropospheric Ozone: processes controlling seasonal variations
South Asia ammonia emission inversion through assimilating IASI observations
Constraining the budget of NOx and VOCs at a remote Tropical island using multi-platform observations and WRF-Chem model simulations
A CO2–Δ14CO2 inversion setup for estimating European fossil CO2 emissions
Maximum ozone concentrations in the southwestern US and Texas: implications of the growing predominance of the background contribution
Derivation of atmospheric reaction mechanisms for volatile organic compounds by the SAPRC mechanism generation system (MechGen)
Comparative ozone production sensitivity to NOx and VOCs in Quito, Ecuador and Santiago, Chile: implications for control strategies in times of climate action
Seasonal, regional, and vertical characteristics of high-carbon-monoxide plumes along with their associated ozone anomalies, as seen by IAGOS between 2002 and 2019
Tropospheric ozone trends and attributions over East and Southeast Asia in 1995–2019: An integrated assessment using statistical methods, machine learning models, and multiple chemical transport models
The potential of drone observations to improve air quality predictions by 4D-Var
Process analysis of elevated concentrations of organic acids at Whiteface Mountain, New York
Sensitivity of climate-chemistry model simulated atmospheric composition to lightning-produced NOx parameterizations based on lightning frequency
Ozone source attribution in polluted European areas during summer 2017 as simulated with MECO(n)
Surface ozone trend variability across the United States and the impact of heatwaves (1990–2023)
Opinion: Challenges and needs of tropospheric chemical mechanism development
Decrease of the European NOx anthropogenic emissions between 2005 and 2019 as seen from the OMI and TROPOMI NO2 satellite observations
Tracking daily NOx emissions from an urban agglomeration based on TROPOMI NO2 and a local ensemble transform Kalman filter
The atmospheric oxidizing capacity in China – Part 2: Sensitivity to emissions of primary pollutants
Role of chemical production and depositional losses on formaldehyde in the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM)
Review of source analyses of ambient volatile organic compounds considering reactive losses: methods of reducing loss effects, impacts of losses, and sources
Interpreting summertime hourly variation of NO2 columns with implications for geostationary satellite applications
An investigation into atmospheric nitrous acid (HONO) processes in South Korea
Soil Deposition of Atmospheric Hydrogen Constrained using Planetary Scale Observations
Performance evaluation of UKESM1 for surface ozone across the pan-tropics
Constraining light dependency in modeled emissions through comparison to observed biogenic volatile organic compound (BVOC) concentrations in a southeastern US forest
A global re-analysis of regionally resolved emissions and atmospheric mole fractions of SF6 for the period 2005–2021
Tropospheric ozone precursors: global and regional distributions, trends, and variability
Representing improved tropospheric ozone distribution by including lightning NOx emissions in CHIMERE
Ragnhild Bieltvedt Skeie, Marit Sandstad, Srinath Krishnan, Gunnar Myhre, and Maria Sand
Atmos. Chem. Phys., 25, 4929–4942, https://doi.org/10.5194/acp-25-4929-2025, https://doi.org/10.5194/acp-25-4929-2025, 2025
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Hydrogen leakages can alter the amount of climate gases in the atmosphere and hence have a climate impact. In this study we investigate, using an atmospheric chemistry model, how this indirect climate effect differs with different amounts of leakages and with where the hydrogen leaks and if this effect changes in the future. The effect is largest for emissions far from areas where hydrogen is removed from the atmosphere by the soil, but these are not relevant locations for a future hydrogen economy.
Alok K. Pandey, David S. Stevenson, Alcide Zhao, Richard J. Pope, Ryan Hossaini, Krishan Kumar, and Martyn P. Chipperfield
Atmos. Chem. Phys., 25, 4785–4802, https://doi.org/10.5194/acp-25-4785-2025, https://doi.org/10.5194/acp-25-4785-2025, 2025
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Nitrogen dioxide is an air pollutant largely controlled by human activity that affects ozone, methane, and aerosols. Satellite instruments can quantify column NO2 and, by carefully matching the time and location of measurements, enable evaluation of model simulations. NO2 over south and east Asia is assessed, showing that the model captures not only many features of the measurements, but also important differences that suggest model deficiencies in representing several aspects of the atmospheric chemistry of NO2.
Mingzhao Liu, Lars Hoffmann, Jens-Uwe Grooß, Zhongyin Cai, Sabine Grießbach, and Yi Heng
Atmos. Chem. Phys., 25, 4403–4418, https://doi.org/10.5194/acp-25-4403-2025, https://doi.org/10.5194/acp-25-4403-2025, 2025
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We studied the transport and chemical decomposition of volcanic SO2, focusing on the 2019 Raikoke event. By comparing two different chemistry modeling schemes, we found that including complex chemical reactions leads to a more accurate prediction of how long SO2 stays in the atmosphere. This research helps improve our understanding of volcanic pollution and its impact on air quality and climate, providing better tools for scientists to track and predict the movement of these pollutants.
Yufen Wang, Ke Li, Xi Chen, Zhenjiang Yang, Minglong Tang, Pascoal M. D. Campos, Yang Yang, Xu Yue, and Hong Liao
Atmos. Chem. Phys., 25, 4455–4475, https://doi.org/10.5194/acp-25-4455-2025, https://doi.org/10.5194/acp-25-4455-2025, 2025
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The impacts of biomass burning and anthropogenic emissions on high tropospheric ozone levels are not well studied in southern Africa. We combined model simulations with recent observations at the surface and from space to quantify tropospheric ozone and its drivers in southern Africa. Our work focuses on the impact of emissions from different sources at different spatial scales, contributing to a comprehensive understanding of air pollution drivers and their uncertainties in southern Africa.
Dominika Pasik, Thomas Golin Almeida, Emelda Ahongshangbam, Siddharth Iyer, and Nanna Myllys
Atmos. Chem. Phys., 25, 4313–4331, https://doi.org/10.5194/acp-25-4313-2025, https://doi.org/10.5194/acp-25-4313-2025, 2025
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We used quantum chemistry methods to investigate the oxidation mechanisms of acyl peroxy radicals (APRs) with various monoterpenes. Our findings reveal unique oxidation pathways for different monoterpenes, leading to either chain-terminating products or highly reactive intermediates that can contribute to particle formation in the atmosphere. This research highlights APRs as potentially significant but underexplored atmospheric oxidants that may influence future approaches to modelling climate.
Jincheol Park, Yunsoo Choi, and Sagun Kayastha
Atmos. Chem. Phys., 25, 4291–4311, https://doi.org/10.5194/acp-25-4291-2025, https://doi.org/10.5194/acp-25-4291-2025, 2025
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We investigated NOx emission contributions to NOy loadings across five regions of East Asia during the 2022 winter–spring transition through chemical transport modeling informed by satellite data. As seasons progress, local contributions within each region to its NOy budget decreased from 32 %–43 % to 23 %–30 %, while transboundary contributions increased from 16 %–33 % to 27 %–37 %, driven by a shift in synoptic settings that allowed pollutants to spread more broadly across the regions.
Qianqian Zhang, K. Folkert Boersma, Chiel van der Laan, Alba Mols, Bin Zhao, Shengyue Li, and Yuepeng Pan
Atmos. Chem. Phys., 25, 3313–3326, https://doi.org/10.5194/acp-25-3313-2025, https://doi.org/10.5194/acp-25-3313-2025, 2025
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Accurate NOx emission estimates are required to better understand air pollution. This study investigates and demonstrates the ability of the superposition column model in combination with TROPOMI tropospheric NO2 column data to estimate city-scale NOx emissions and lifetimes and their variabilities. The results of this work nevertheless confirm the strength of the superposition column model in estimating urban NOx emissions with reasonable accuracy.
Wenbin Kou, Yang Gao, Dan Tong, Xiaojie Guo, Xiadong An, Wenyu Liu, Mengshi Cui, Xiuwen Guo, Shaoqing Zhang, Huiwang Gao, and Lixin Wu
Atmos. Chem. Phys., 25, 3029–3048, https://doi.org/10.5194/acp-25-3029-2025, https://doi.org/10.5194/acp-25-3029-2025, 2025
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Unlike traditional numerical studies, we apply a high-resolution Earth system model, improving simulations of surface ozone and large-scale circulations such as atmospheric blocking. Besides local heat waves, we quantify the impact of atmospheric blocking on downstream ozone concentrations, which is closely associated with the blocking position. We identify three major pathways of Rossby wave propagation, stressing the critical role of large-scale circulation in regional air quality.
Beata Opacka, Trissevgeni Stavrakou, Jean-François Müller, Isabelle De Smedt, Jos van Geffen, Eloise A. Marais, Rebekah P. Horner, Dylan B. Millet, Kelly C. Wells, and Alex B. Guenther
Atmos. Chem. Phys., 25, 2863–2894, https://doi.org/10.5194/acp-25-2863-2025, https://doi.org/10.5194/acp-25-2863-2025, 2025
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Vegetation releases biogenic volatile organic compounds, while soils and lightning contribute to the natural emissions of nitrogen oxides into the atmosphere. These gases interact in complex ways. Using satellite data and models, we developed a new method to simultaneously optimize these natural emissions over Africa in 2019. Our approach resulted in an increase in natural emissions, supported by independent data indicating that current estimates are underestimated.
Shuai Li, Haolin Wang, and Xiao Lu
Atmos. Chem. Phys., 25, 2725–2743, https://doi.org/10.5194/acp-25-2725-2025, https://doi.org/10.5194/acp-25-2725-2025, 2025
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Summertime ozone–temperature sensitivity has decreased by 50 % from 3.0 ppbv per K in 1990 to 1.5 ppb per K in 2021 in the US. GEOS-Chem simulations show that anthropogenic nitrogen oxide emission reduction is the dominant driver of ozone–temperature sensitivity decline by influencing both temperature direct and temperature indirect processes. Reduced ozone–temperature sensitivity has decreased ozone enhancement from low to high temperatures by an average of 6.8 ppbv across the US.
Jinya Yang, Yutong Wang, Lei Zhang, and Yu Zhao
Atmos. Chem. Phys., 25, 2649–2666, https://doi.org/10.5194/acp-25-2649-2025, https://doi.org/10.5194/acp-25-2649-2025, 2025
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We develop a modeling framework to predict future ozone concentrations (till the 2060s) in China following an IPCC scenario. We evaluate the contributions of climatic, anthropogenic, and biogenic factors by season and region. We find persistent emission controls will alter the nonlinear response of ozone to its precursors and dominate the declining ozone level. The outcomes highlight the importance of human actions, even with a climate penalty on air quality.
Takashi Sekiya, Emanuele Emili, Kazuyuki Miyazaki, Antje Inness, Zhen Qu, R. Bradley Pierce, Dylan Jones, Helen Worden, William Y. Y. Cheng, Vincent Huijnen, and Gerbrand Koren
Atmos. Chem. Phys., 25, 2243–2268, https://doi.org/10.5194/acp-25-2243-2025, https://doi.org/10.5194/acp-25-2243-2025, 2025
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Five global chemical reanalysis datasets were used to assess the relative impacts of assimilating satellite ozone and its precursor measurements on tropospheric ozone analyses for 2010. The multiple reanalysis system comparison allows an evaluation of the dependency of the impacts on different reanalysis systems. The results suggested the importance of satellite ozone and its precursor measurements for improving ozone analysis in the whole troposphere, with varying magnitudes among the systems.
Maureen Beaudor, Didier Hauglustaine, Juliette Lathière, Martin Van Damme, Lieven Clarisse, and Nicolas Vuichard
Atmos. Chem. Phys., 25, 2017–2046, https://doi.org/10.5194/acp-25-2017-2025, https://doi.org/10.5194/acp-25-2017-2025, 2025
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Agriculture is the biggest ammonia (NH3) source, impacting air quality, climate, and ecosystems. Because of food demand, NH3 emissions are projected to rise by 2100. Using a global model, we analyzed the impact of present and future NH3 emissions generated from a land model. Our results show improved ammonia patterns compared to a reference inventory. Future scenarios predict up to 70 % increase in global NH3 burden, with significant changes in radiative forcing that can greatly elevate N2O.
Hui Li, Jiaxin Qiu, and Bo Zheng
Atmos. Chem. Phys., 25, 1949–1963, https://doi.org/10.5194/acp-25-1949-2025, https://doi.org/10.5194/acp-25-1949-2025, 2025
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We conduct a sensitivity analysis with 31 tests on various factors including prior emissions, model resolution, satellite constraint, and other system configurations to assess the vulnerability of emission estimates across temporal, sectoral, and regional dimensions. This reveals the robustness of emissions estimated by this air-pollution-satellite-based CO2 emission inversion system, with relative change between tests and base inversion below 4.0 % for national annual NOx and CO2 emissions.
Yuqing Qiu, Xin Li, Wenxuan Chai, Yi Liu, Mengdi Song, Xudong Tian, Qiaoli Zou, Wenjun Lou, Wangyao Zhang, Juan Li, and Yuanhang Zhang
Atmos. Chem. Phys., 25, 1749–1763, https://doi.org/10.5194/acp-25-1749-2025, https://doi.org/10.5194/acp-25-1749-2025, 2025
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The chemical reactions of ozone (O3) formation are related to meteorology and local emissions. Here, a random forest approach was used to eliminate the effects of meteorological factors (dispersion or transport) on O3 and its precursors. Variations in the sensitivity of O3 formation and the apportionment of emission sources were revealed after meteorological normalization. Our results suggest that meteorological variations should be considered when diagnosing O3 formation.
Jeongmin Yun, Junjie Liu, Brendan Byrne, Brad Weir, Lesley E. Ott, Kathryn McKain, Bianca C. Baier, Luciana V. Gatti, and Sebastien C. Biraud
Atmos. Chem. Phys., 25, 1725–1748, https://doi.org/10.5194/acp-25-1725-2025, https://doi.org/10.5194/acp-25-1725-2025, 2025
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This study quantifies errors in regional net surface–atmosphere CO2 flux estimates from an inverse model ensemble using airborne CO2 measurements. Our results show that flux error estimates based on observations significantly exceed those computed from the ensemble spread of flux estimates in regions with high fossil fuel emissions. This finding suggests the presence of systematic biases in the inversion estimates, associated with errors in the fossil fuel emissions common to all models.
Min Huang, Gregory R. Carmichael, Kevin W. Bowman, Isabelle De Smedt, Andreas Colliander, Michael H. Cosh, Sujay V. Kumar, Alex B. Guenther, Scott J. Janz, Ryan M. Stauffer, Anne M. Thompson, Niko M. Fedkin, Robert J. Swap, John D. Bolten, and Alicia T. Joseph
Atmos. Chem. Phys., 25, 1449–1476, https://doi.org/10.5194/acp-25-1449-2025, https://doi.org/10.5194/acp-25-1449-2025, 2025
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We use model simulations along with multiplatform, multidisciplinary observations and a range of analysis methods to estimate and understand the distributions, temporal changes, and impacts of reactive nitrogen and ozone over the most populous US region that has undergone significant environmental changes. Deposition, biogenic emissions, and extra-regional sources have been playing increasingly important roles in controlling pollutant budgets in this area as local anthropogenic emissions drop.
Xavier Faïn, Sophie Szopa, Vaishali Naïk, Patricia Martinerie, David M. Etheridge, Rachael H. Rhodes, Cathy M. Trudinger, Vasilii V. Petrenko, Kévin Fourteau, and Philip Place
Atmos. Chem. Phys., 25, 1105–1119, https://doi.org/10.5194/acp-25-1105-2025, https://doi.org/10.5194/acp-25-1105-2025, 2025
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Carbon monoxide (CO) plays a crucial role in the atmosphere's oxidizing capacity. In this study, we analyse how historical (1850–2014) [CO] outputs from state-of-the-art global chemistry–climate models over Greenland and Antarctica are able to capture both absolute values and trends recorded in multi-site ice archives. A disparity in [CO] growth rates emerges in the Northern Hemisphere between models and observations from 1920–1975 CE, possibly linked to uncertainties in CO emission factors.
Natalie Brett, Kathy S. Law, Steve R. Arnold, Javier G. Fochesatto, Jean-Christophe Raut, Tatsuo Onishi, Robert Gilliam, Kathleen Fahey, Deanna Huff, George Pouliot, Brice Barret, Elsa Dieudonné, Roman Pohorsky, Julia Schmale, Andrea Baccarini, Slimane Bekki, Gianluca Pappaccogli, Federico Scoto, Stefano Decesari, Antonio Donateo, Meeta Cesler-Maloney, William Simpson, Patrice Medina, Barbara D'Anna, Brice Temime-Roussel, Joel Savarino, Sarah Albertin, Jingqiu Mao, Becky Alexander, Allison Moon, Peter F. DeCarlo, Vanessa Selimovic, Robert Yokelson, and Ellis S. Robinson
Atmos. Chem. Phys., 25, 1063–1104, https://doi.org/10.5194/acp-25-1063-2025, https://doi.org/10.5194/acp-25-1063-2025, 2025
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Processes influencing dispersion of local anthropogenic pollution in Arctic wintertime are investigated with Lagrangian dispersion modelling. Simulated power plant plume rise that considers temperature inversion layers improves results compared to observations (interior Alaska). Modelled surface concentrations are improved by representation of vertical mixing and emission estimates. Large increases in diesel vehicle emissions at temperatures reaching −35°C are required to reproduce observed NOx.
Chelsea E. Stockwell, Matthew M. Coggon, Rebecca H. Schwantes, Colin Harkins, Bert Verreyken, Congmeng Lyu, Qindan Zhu, Lu Xu, Jessica B. Gilman, Aaron Lamplugh, Jeff Peischl, Michael A. Robinson, Patrick R. Veres, Meng Li, Andrew W. Rollins, Kristen Zuraski, Sunil Baidar, Shang Liu, Toshihiro Kuwayama, Steven S. Brown, Brian C. McDonald, and Carsten Warneke
Atmos. Chem. Phys., 25, 1121–1143, https://doi.org/10.5194/acp-25-1121-2025, https://doi.org/10.5194/acp-25-1121-2025, 2025
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In urban areas, emissions from everyday products like paints, cleaners, and personal care products, along with non-traditional sources such as cooking, are increasingly important and impact air quality. This study uses a box model to evaluate how these emissions impact ozone in the Los Angeles Basin and quantifies the impact of gaseous cooking emissions. Accurate representation of these and other anthropogenic sources in inventories is crucial for informing effective air quality policies.
Xiaodan Ma, Jianping Huang, Michaela I. Hegglin, Patrick Jöckel, and Tianliang Zhao
Atmos. Chem. Phys., 25, 943–958, https://doi.org/10.5194/acp-25-943-2025, https://doi.org/10.5194/acp-25-943-2025, 2025
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Our research explored changes in ozone levels in the northwest Pacific region over 30 years, revealing a significant increase in the middle-to-upper troposphere, especially during spring and summer. This rise is influenced by both stratospheric and tropospheric sources, which affect climate and air quality in East Asia. This work underscores the need for continued study to understand underlying mechanisms.
Hiroo Hata, Norifumi Mizushima, and Tomohiko Ihara
Atmos. Chem. Phys., 25, 1037–1061, https://doi.org/10.5194/acp-25-1037-2025, https://doi.org/10.5194/acp-25-1037-2025, 2025
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The introduction of battery electric vehicles (BEVs) is expected to reduce the primary air pollutants from vehicular exhaust and evaporative emissions while reducing the anthropogenic heat produced by vehicles, ultimately mitigating the urban heat island (UHI) effect. This study revealed the impact of introducing BEVs on the decrease in the UHI effect and the impact of BEVs on the formation of tropospheric ozone and fine particulate matter in the Greater Tokyo Area of Japan.
Wanmin Gong, Stephen R. Beagley, Kenjiro Toyota, Henrik Skov, Jesper Heile Christensen, Alexandru Lupu, Diane Pendlebury, Junhua Zhang, Ulas Im, Yugo Kanaya, Alfonso Saiz-Lopez, Roberto Sommariva, Peter Effertz, John W. Halfacre, Nis Jepsen, Rigel Kivi, Theodore K. Koenig, Katrin Müller, Claus Nordstrøm, Irina Petropavlovskikh, Paul B. Shepson, William R. Simpson, Sverre Solberg, Ralf M. Staebler, David W. Tarasick, Roeland Van Malderen, and Mika Vestenius
EGUsphere, https://doi.org/10.5194/egusphere-2024-3750, https://doi.org/10.5194/egusphere-2024-3750, 2025
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This study showed that the springtime O3 depletion plays a critical role in driving the surface O3 seasonal cycle in Central Arctic. The O3 depletion events, while occurring most notably within the lowest few hundred metres above the Arctic Ocean, can induce a 5–7 % of loss in the pan-Arctic tropospheric O3 burden during springtime. The study also found an enhancement in O3 and NOy (mostly PAN) concentrations in the Arctic due to northern boreal wildfires, particularly at altitudes.
Ji Xia, Yi Zhou, Li Fang, Yingfei Qi, Dehao Li, Hong Liao, and Jianbing Jin
EGUsphere, https://doi.org/10.5194/egusphere-2024-3938, https://doi.org/10.5194/egusphere-2024-3938, 2025
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This study established an ammonia emission inventory in South Asia via assimilation-based inversion system. The posterior emissions, calculated by integrating the CEDS inventory and IASI satellite observations, showed significant improvement over the prior. Validation against various measurements all support our posterior emission. It offers valuable insights of ammonia emissions for policymakers and researchers aiming to develop air quality management and mitigation strategies there.
Catalina Poraicu, Jean-François Müller, Trissevgeni Stavrakou, Crist Amelynck, Bert W. D. Verreyken, Niels Schoon, Corinne Vigouroux, Nicolas Kumps, Jérôme Brioude, Pierre Tulet, and Camille Mouchel-Vallon
EGUsphere, https://doi.org/10.5194/egusphere-2024-3555, https://doi.org/10.5194/egusphere-2024-3555, 2025
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We investigated the sources and impacts of nitrogen oxides and organic compounds over a remote tropical island. High-resolution WRF-Chem simulations were evaluated using in situ, FTIR and satellite measurements. This work highlights gaps in current models, like missing sources of key organic compounds and inaccuracies in emission inventories, emphasizing the importance of improving chemical and dynamical processes in atmospheric modelling for budget estimates in tropical regions.
Carlos Gómez-Ortiz, Guillaume Monteil, Sourish Basu, and Marko Scholze
Atmos. Chem. Phys., 25, 397–424, https://doi.org/10.5194/acp-25-397-2025, https://doi.org/10.5194/acp-25-397-2025, 2025
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In this paper, we test new implementations of our inverse modeling tool to estimate the weekly and regional CO2 emissions from fossil fuels in Europe. We use synthetic atmospheric observations of CO2 and radiocarbon (14CO2) to trace emissions to their sources, while separating the natural and fossil CO2. Our tool accurately estimates fossil CO2 emissions in densely monitored regions like western/central Europe. This approach aids in developing strategies for reducing CO2 emissions.
David D. Parrish, Ian C. Faloona, and Richard G. Derwent
Atmos. Chem. Phys., 25, 263–289, https://doi.org/10.5194/acp-25-263-2025, https://doi.org/10.5194/acp-25-263-2025, 2025
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Observation-based estimates of contributions to maximum ozone (O3) concentrations show that background O3 can exceed the air quality standard of 70 ppb in the southwestern US, precluding standard attainment. Over the past 4 decades, US anthropogenic O3 has decreased by a factor of ~ 6.3, while wildfire contributions have increased, so that the background now dominates maximum concentrations, even in Los Angeles, and the occurrence of maximum O3 has shifted from the eastern to the western US.
William P. L. Carter, Jia Jiang, John J. Orlando, and Kelley C. Barsanti
Atmos. Chem. Phys., 25, 199–242, https://doi.org/10.5194/acp-25-199-2025, https://doi.org/10.5194/acp-25-199-2025, 2025
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This paper describes the scientific basis for gas-phase atmospheric chemical mechanisms derived using the SAPRC mechanism generation system, MechGen. It can derive mechanisms for most organic compounds with C, H, O, or N atoms, including initial reactions of organics with OH, O3, NO3, and O3P or by photolysis, as well as the reactions of the various types of intermediates that are formed. The paper includes a description of areas of uncertainty where additional research and updates are needed.
María Cazorla, Melissa Trujillo, Rodrigo Seguel, and Laura Gallardo
EGUsphere, https://doi.org/10.5194/egusphere-2024-3720, https://doi.org/10.5194/egusphere-2024-3720, 2024
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The current climate emergency imposes the need to take actions in cities to curb ozone as a pollutant and a climate forcer. In this work we analyze how reducing the levels of ozone precursor would affect photochemical smog in Quito, Ecuador and Santiago, Chile. Results show that if environmental policy were implemented to reduce only nitrogen oxides, the production of ozone would increase substantially for which more integral solutions are needed.
Thibaut Lebourgeois, Bastien Sauvage, Pawel Wolff, Béatrice Josse, Virginie Marécal, Yasmine Bennouna, Romain Blot, Damien Boulanger, Hannah Clark, Jean-Marc Cousin, Philippe Nedelec, and Valérie Thouret
Atmos. Chem. Phys., 24, 13975–14004, https://doi.org/10.5194/acp-24-13975-2024, https://doi.org/10.5194/acp-24-13975-2024, 2024
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Our study examines intense-carbon-monoxide (CO) pollution events measured by commercial aircraft from the In-service Aircraft for a Global Observing System (IAGOS) research infrastructure. We combine these measurements with the SOFT-IO model to trace the origin of the observed CO. A comprehensive analysis of the geographical origin, source type, seasonal variation, and ozone levels of these pollution events is provided.
Xiao Lu, Yiming Liu, Jiayin Su, Xiang Weng, Tabish Ansari, Yuqiang Zhang, Guowen He, Yuqi Zhu, Haolin Wang, Ganquan Zeng, Jingyu Li, Cheng He, Shuai Li, Teerachai Amnuaylojaroen, Tim Butler, Qi Fan, Shaojia Fan, Grant L. Forster, Meng Gao, Jianlin Hu, Yugo Kanaya, Mohd Talib Latif, Keding Lu, Philippe Nédélec, Peer Nowack, Bastien Sauvage, Xiaobin Xu, Lin Zhang, Ke Li, Ja-Ho Koo, and Tatsuya Nagashima
EGUsphere, https://doi.org/10.5194/egusphere-2024-3702, https://doi.org/10.5194/egusphere-2024-3702, 2024
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This study analyzes summertime ozone trends in East and Southeast Asia derived from a comprehensive observational database spanning from 1995 to 2019, incorporating aircraft observations, ozonesonde data, and measurements from 2500 surface sites. Multiple models are applied to attribute to changes in anthropogenic emissions and climate. The results highlight increases in anthropogenic emission are the primary driver of ozone increases both in the free troposphere and at the surface.
Hassnae Erraji, Philipp Franke, Astrid Lampert, Tobias Schuldt, Ralf Tillmann, Andreas Wahner, and Anne Caroline Lange
Atmos. Chem. Phys., 24, 13913–13934, https://doi.org/10.5194/acp-24-13913-2024, https://doi.org/10.5194/acp-24-13913-2024, 2024
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Four-dimensional variational data assimilation allows for the simultaneous optimisation of initial values and emission rates by using trace-gas profiles from drone observations in a regional air quality model. Assimilated profiles positively impact the representation of air pollutants in the model by improving their vertical distribution and ground-level concentrations. This case study highlights the potential of drone data to enhance air quality analyses including local emission evaluation.
Christopher Lawrence, Mary Barth, John Orlando, Paul Casson, Richard Brandt, Daniel Kelting, Elizabeth Yerger, and Sara Lance
Atmos. Chem. Phys., 24, 13693–13713, https://doi.org/10.5194/acp-24-13693-2024, https://doi.org/10.5194/acp-24-13693-2024, 2024
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This work uses chemical transport and box modeling to study the gas- and aqueous-phase production of organic acid concentrations measured in cloud water at the summit of Whiteface Mountain on 1 July 2018. Isoprene was the major source of formic, acetic, and oxalic acid. Gas-phase chemistry greatly underestimated formic and acetic acid, indicating missing sources, while cloud chemistry was a key source of oxalic acid. More studies of organic acids are required to better constrain their sources.
Francisco J. Pérez-Invernón, Francisco J. Gordillo-Vázquez, Heidi Huntrieser, Patrick Jöckel, and Eric J. Bucsela
EGUsphere, https://doi.org/10.5194/egusphere-2024-3348, https://doi.org/10.5194/egusphere-2024-3348, 2024
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Lightning plays a significant role in tropospheric chemistry by producing substantial amounts of nitrogen oxides. According to recent estimates, thunderstorms that produce a higher lightning frequency rate also produce less nitrogen oxide per flash. We implemented the dependency of nitrogen oxide production per flash on lightning flash frequency in a chemical atmospheric model.
Markus Kilian, Volker Grewe, Patrick Jöckel, Astrid Kerkweg, Mariano Mertens, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 24, 13503–13523, https://doi.org/10.5194/acp-24-13503-2024, https://doi.org/10.5194/acp-24-13503-2024, 2024
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Anthropogenic emissions are a major source of precursors of tropospheric ozone. As ozone formation is highly non-linear, we apply a global–regional chemistry–climate model with a source attribution method (tagging) to quantify the contribution of anthropogenic emissions to ozone. Our analysis shows that the contribution of European anthropogenic emissions largely increases during large ozone periods, indicating that emissions from these sectors drive ozone values.
Kai-Lan Chang, Brian C. McDonald, and Owen R. Cooper
EGUsphere, https://doi.org/10.5194/egusphere-2024-3674, https://doi.org/10.5194/egusphere-2024-3674, 2024
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Exposure to high levels of ozone can be harmful to human health. This study shows consistent and robust evidence of decreasing ozone extremes across much of the United States over 1990–2023, previously attributed to ozone precursor emission controls. Nevertheless, we also show that the increasing heatwave frequencies are likely to contribute to additional ozone exceedances, slowing the progress of decreasing the frequency of ozone exceedances.
Barbara Ervens, Andrew Rickard, Bernard Aumont, William P. L. Carter, Max McGillen, Abdelwahid Mellouki, John Orlando, Bénédicte Picquet-Varrault, Paul Seakins, William R. Stockwell, Luc Vereecken, and Timothy J. Wallington
Atmos. Chem. Phys., 24, 13317–13339, https://doi.org/10.5194/acp-24-13317-2024, https://doi.org/10.5194/acp-24-13317-2024, 2024
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Chemical mechanisms describe the chemical processes in atmospheric models that are used to describe the changes in the atmospheric composition. Therefore, accurate chemical mechanisms are necessary to predict the evolution of air pollution and climate change. The article describes all steps that are needed to build chemical mechanisms and discusses the advances and needs of experimental and theoretical research activities needed to build reliable chemical mechanisms.
Audrey Fortems-Cheiney, Grégoire Broquet, Robin Plauchu, Elise Potier, Antoine Berchet, Isabelle Pison, Adrien Martinez, Rimal Abeed, Gaelle Dufour, Adriana Coman, Dilek Savas, Guillaume Siour, Henk Eskes, Hugo A. C. Denier van der Gon, and Stijn N. C. Dellaert
EGUsphere, https://doi.org/10.5194/egusphere-2024-3679, https://doi.org/10.5194/egusphere-2024-3679, 2024
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This study assesses the potential of the OMI and TROPOMI satellite observations to inform about the evolution of NOx anthropogenic emissions between year 2005 and year 2019 at the regional to national scales in Europe. Both the OMI and TROPOMI inversions show decreases in European NOx anthropogenic emission budgets between 2005 and 2019, but with different magnitudes.
Yawen Kong, Bo Zheng, and Yuxi Liu
EGUsphere, https://doi.org/10.5194/egusphere-2024-2996, https://doi.org/10.5194/egusphere-2024-2996, 2024
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Current high-resolution satellite remote sensing technologies provide a unique opportunity to derive timely, high-resolution emission data. We developed an emission inversion system to assimilate satellite NO2 data to obtain daily, kilometer-scale NOx emission inventories. Our results enhance inventory accuracy, allowing us to capture the effects of pollution control policies on daily emissions (e.g., during COVID-19 lockdown) and improve fine-scale air quality modeling.
Jianing Dai, Guy P. Brasseur, Mihalis Vrekoussis, Maria Kanakidou, Kun Qu, Yijuan Zhang, Hongliang Zhang, and Tao Wang
Atmos. Chem. Phys., 24, 12943–12962, https://doi.org/10.5194/acp-24-12943-2024, https://doi.org/10.5194/acp-24-12943-2024, 2024
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This paper employs a regional chemical transport model to quantify the sensitivity of air pollutants and photochemical parameters to specified emission reductions in China for representative winter and summer conditions. The study provides insights into further air quality control in China with reduced primary emissions.
T. Nash Skipper, Emma L. D'Ambro, Forwood C. Wiser, V. Faye McNeill, Rebecca H. Schwantes, Barron H. Henderson, Ivan R. Piletic, Colleen B. Baublitz, Jesse O. Bash, Andrew R. Whitehill, Lukas C. Valin, Asher P. Mouat, Jennifer Kaiser, Glenn M. Wolfe, Jason M. St. Clair, Thomas F. Hanisco, Alan Fried, Bryan K. Place, and Havala O.T. Pye
Atmos. Chem. Phys., 24, 12903–12924, https://doi.org/10.5194/acp-24-12903-2024, https://doi.org/10.5194/acp-24-12903-2024, 2024
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We develop the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM) version 2 to improve predictions of formaldehyde in ambient air compared to satellite-, aircraft-, and ground-based observations. With the updated chemistry, we estimate the cancer risk from inhalation exposure to ambient formaldehyde across the contiguous USA and predict that 40 % of this risk is controllable through reductions in anthropogenic emissions of nitrogen oxides and reactive organic carbon.
Baoshuang Liu, Yao Gu, Yutong Wu, Qili Dai, Shaojie Song, Yinchang Feng, and Philip K. Hopke
Atmos. Chem. Phys., 24, 12861–12879, https://doi.org/10.5194/acp-24-12861-2024, https://doi.org/10.5194/acp-24-12861-2024, 2024
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Reactive loss of volatile organic compounds (VOCs) is a long-term issue yet to be resolved in VOC source analyses. We assess common methods of, and existing issues in, reducing losses, impacts of losses, and sources in current source analyses. We offer a potential supporting role for solving issues of VOC conversion. Source analyses of consumed VOCs that reacted to produce ozone and secondary organic aerosols can play an important role in the effective control of secondary pollution in air.
Deepangsu Chatterjee, Randall V. Martin, Chi Li, Dandan Zhang, Haihui Zhu, Daven K. Henze, James H. Crawford, Ronald C. Cohen, Lok N. Lamsal, and Alexander M. Cede
Atmos. Chem. Phys., 24, 12687–12706, https://doi.org/10.5194/acp-24-12687-2024, https://doi.org/10.5194/acp-24-12687-2024, 2024
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We investigate the hourly variation of NO2 columns and surface concentrations by applying the GEOS-Chem model to interpret aircraft and ground-based measurements over the US and Pandora sun photometer measurements over the US, Europe, and Asia. Corrections to the Pandora columns and finer model resolution improve the modeled representation of the summertime hourly variation of total NO2 columns to explain the weaker hourly variation in NO2 columns than at the surface.
Kiyeon Kim, Kyung Man Han, Chul Han Song, Hyojun Lee, Ross Beardsley, Jinhyeok Yu, Greg Yarwood, Bonyoung Koo, Jasper Madalipay, Jung-Hun Woo, and Seogju Cho
Atmos. Chem. Phys., 24, 12575–12593, https://doi.org/10.5194/acp-24-12575-2024, https://doi.org/10.5194/acp-24-12575-2024, 2024
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We incorporated each HONO process into the current CMAQ modeling framework to enhance the accuracy of HONO mixing ratio predictions. These results expand our understanding of HONO photochemistry and identify crucial sources of HONO that impact the total HONO budget in Seoul, South Korea. Through this investigation, we contribute to resolving discrepancies in understanding chemical transport models, with implications for better air quality management and environmental protection in the region.
Alexander Karim Tardito Chaudhri and David S. Stevenson
EGUsphere, https://doi.org/10.5194/egusphere-2024-3247, https://doi.org/10.5194/egusphere-2024-3247, 2024
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There remains a large uncertainty in the global warming potential of atmospheric hydrogen due to poor constraints on its soil deposition, and therefore its lifetime. A new analysis of the latitudinal variation in the observed seasonality of hydrogen is used to constrain its surface fluxes. This is complemented with a simple latitude-height model where surface fluxes are adjusted from a prototype deposition scheme.
Flossie Brown, Gerd Folberth, Stephen Sitch, Paulo Artaxo, Marijn Bauters, Pascal Boeckx, Alexander W. Cheesman, Matteo Detto, Ninong Komala, Luciana Rizzo, Nestor Rojas, Ines dos Santos Vieira, Steven Turnock, Hans Verbeeck, and Alfonso Zambrano
Atmos. Chem. Phys., 24, 12537–12555, https://doi.org/10.5194/acp-24-12537-2024, https://doi.org/10.5194/acp-24-12537-2024, 2024
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Ozone is a pollutant that is detrimental to human and plant health. Ozone monitoring sites in the tropics are limited, so models are often used to understand ozone exposure. We use measurements from the tropics to evaluate ozone from the UK Earth system model, UKESM1. UKESM1 is able to capture the pattern of ozone in the tropics, except in southeast Asia, although it systematically overestimates it at all sites. This work highlights that UKESM1 can capture seasonal and hourly variability.
Namrata Shanmukh Panji, Deborah F. McGlynn, Laura E. R. Barry, Todd M. Scanlon, Manuel T. Lerdau, Sally E. Pusede, and Gabriel Isaacman-VanWertz
Atmos. Chem. Phys., 24, 12495–12507, https://doi.org/10.5194/acp-24-12495-2024, https://doi.org/10.5194/acp-24-12495-2024, 2024
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Climate change will bring about changes in parameters that are currently used in global-scale models to calculate biogenic emissions. This study seeks to understand the factors driving these models by comparing long-term datasets of biogenic compounds to modeled emissions. We note that the light-dependent fractions currently used in models do not accurately represent regional observations. We provide evidence for the time-dependent variation in this parameter for future modifications to models.
Martin Vojta, Andreas Plach, Saurabh Annadate, Sunyoung Park, Gawon Lee, Pallav Purohit, Florian Lindl, Xin Lan, Jens Mühle, Rona L. Thompson, and Andreas Stohl
Atmos. Chem. Phys., 24, 12465–12493, https://doi.org/10.5194/acp-24-12465-2024, https://doi.org/10.5194/acp-24-12465-2024, 2024
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We constrain the global emissions of the very potent greenhouse gas sulfur hexafluoride (SF6) between 2005 and 2021. We show that SF6 emissions are decreasing in the USA and in the EU, while they are substantially growing in China, leading overall to an increasing global emission trend. The national reports for the USA, EU, and China all underestimated their SF6 emissions. However, stringent mitigation measures can successfully reduce SF6 emissions, as can be seen in the EU emission trend.
Yasin Elshorbany, Jerald R. Ziemke, Sarah Strode, Hervé Petetin, Kazuyuki Miyazaki, Isabelle De Smedt, Kenneth Pickering, Rodrigo J. Seguel, Helen Worden, Tamara Emmerichs, Domenico Taraborrelli, Maria Cazorla, Suvarna Fadnavis, Rebecca R. Buchholz, Benjamin Gaubert, Néstor Y. Rojas, Thiago Nogueira, Thérèse Salameh, and Min Huang
Atmos. Chem. Phys., 24, 12225–12257, https://doi.org/10.5194/acp-24-12225-2024, https://doi.org/10.5194/acp-24-12225-2024, 2024
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We investigated tropospheric ozone spatial variability and trends from 2005 to 2019 and related those to ozone precursors on global and regional scales. We also investigate the spatiotemporal characteristics of the ozone formation regime in relation to ozone chemical sources and sinks. Our analysis is based on remote sensing products of the tropospheric column of ozone and its precursors, nitrogen dioxide, formaldehyde, and total column CO, as well as ozonesonde data and model simulations.
Sanhita Ghosh, Arineh Cholakian, Sylvain Mailler, and Laurent Menut
EGUsphere, https://doi.org/10.5194/egusphere-2024-3087, https://doi.org/10.5194/egusphere-2024-3087, 2024
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In the study, we estimate the emissions of nitrogen oxides from lightning (LNOx) over the northern hemisphere and study its impact on tropospheric ozone (O3). We evaluate the present state of modelling the lightning, using a classical parametrization scheme and the model CHIMERE. The comparison of the simulated O3 to measurements shows that the inclusion of LNOx emissions remarkably improves the tropospheric O3 distribution, reducing the bias significantly, particularly in the free troposphere.
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