Articles | Volume 24, issue 14
https://doi.org/10.5194/acp-24-8243-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-24-8243-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
22 Jul 2024
Research article |
| 22 Jul 2024
| 22 Jul 2024
Evaluating NOx stack plume emissions using a high-resolution atmospheric chemistry model and satellite-derived NO2 columns
Meteorology and Air Quality, Wageningen University & Research, Wageningen, the Netherlands
Institute for Marine and Atmospheric Research Utrecht (IMAU), Utrecht University, Utrecht, the Netherlands
Bart van Stratum
Meteorology and Air Quality, Wageningen University & Research, Wageningen, the Netherlands
Isidora Anglou
Meteorology and Air Quality, Wageningen University & Research, Wageningen, the Netherlands
Satellite Observations, Royal Netherlands Meteorological Institute, De Bilt, the Netherlands
Klaas Folkert Boersma
Meteorology and Air Quality, Wageningen University & Research, Wageningen, the Netherlands
Satellite Observations, Royal Netherlands Meteorological Institute, De Bilt, the Netherlands
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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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Ara Cho, Linda M. J. Kooijmans, Kukka-Maaria Kohonen, Richard Wehr, and Maarten C. Krol
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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
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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.
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
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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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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.
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).
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.
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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Hong Zhao, Han Dolman, Jan Elbers, Wilma Jans, Bart Kruijt, Eddy Moors, Henk Snellen, Jordi Vila-Guerau de Arellano, Wouter Peters, Maarten Krol, Ronald Hutjes, and Michiel van der Molen
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2025-372, https://doi.org/10.5194/essd-2025-372, 2025
Preprint under review for ESSD
Short summary
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Under the Kyoto Protocol the carbon dioxide (CO2) balance for forest ecosystems was required to be measured. Consequently, CO2 flux measurements have been conducted in Loobos site in the Netherlands since 1996, becoming one of the 17 first FLUXNET sites globally. This paper provides a comprehensive overview of the instrumentation, data processing and the resulting data archive, enabling its further use in data analysis, model development and validation of satellite data retrievals.
Mary Rose Mangan, Jordi Vilà-Guerau de Arellano, Bart J. H. van Stratum, Marie Lothon, Guylaine Canut-Rocafort, and Oscar K. Hartogensis
Atmos. Chem. Phys., 25, 8959–8981, https://doi.org/10.5194/acp-25-8959-2025, https://doi.org/10.5194/acp-25-8959-2025, 2025
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Suvarna Fadnavis, Yasin Elshorbany, Jerald Ziemke, Brice Barret, Alexandru Rap, P. R. Satheesh Chandran, Richard J. Pope, Vijay Sagar, Domenico Taraborrelli, Eric Le Flochmoen, Juan Cuesta, Catherine Wespes, Folkert Boersma, Isolde Glissenaar, Isabelle De Smedt, Michel Van Roozendael, Hervé Petetin, and Isidora Anglou
Atmos. Chem. Phys., 25, 8229–8254, https://doi.org/10.5194/acp-25-8229-2025, https://doi.org/10.5194/acp-25-8229-2025, 2025
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Satellites and model simulations show enhancement in tropospheric ozone, which is highly impacted by human-produced nitrous oxides compared to volatile organic compounds. The increased amount of ozone enhances ozone radiative forcing. The ozone enhancement and associated radiative forcing are the highest over South and East Asia. The emissions of nitrous oxides show a higher influence on shifting ozone photochemical regimes than volatile organic compounds.
Arseniy Karagodin-Doyennel, Fredrik Jansson, Bart J. H. van Stratum, Hugo Denier van der Gon, Jordi Vilà-Guerau de Arellano, and Sander Houweling
Geosci. Model Dev., 18, 4571–4599, https://doi.org/10.5194/gmd-18-4571-2025, https://doi.org/10.5194/gmd-18-4571-2025, 2025
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We introduce a new simulation platform based on the Dutch Atmospheric Large-Eddy Simulation (DALES) to simulate carbon dioxide (CO2) emissions and their dispersion in turbulent environments at a hectometer resolution. This model incorporates both anthropogenic emission inventories and online ecosystem fluxes. Simulation results for the main urban area in the Netherlands demonstrate the strong potential of DALES to improve CO2 emission modeling and to support mitigation strategies.
Alessandro Zanchetta, Steven van Heuven, Joram Hooghiem, Rigel Kivi, Thomas Laemmel, Michel Ramonet, Markus Leuenberger, Peter Nyfeler, Sophia Louise Baartman, Maarten Krol, and Huilin Chen
EGUsphere, https://doi.org/10.5194/egusphere-2025-3079, https://doi.org/10.5194/egusphere-2025-3079, 2025
Short summary
Short summary
Continuous vertical profiles and discrete stratospheric samples of carbonyl sulfide (COS) were collected deploying the balloon-borne AirCore, LISA and BigLISA samplers and measured on a Quantum Cascade Laser Spectrometer (QCLS). Our measurements show good accordance with previous COS observations. Moreover, laboratory tests of ozone (O3) scrubbers proved squalene to remove O3 very efficiently without biasing the measurements of other trace gases.
Getachew Agmuas Adnew, Gerbrand Koren, Neha Mehendale, Sergey Gromov, Maarten Krol, and Thomas Röckmann
Atmos. Meas. Tech., 18, 2701–2719, https://doi.org/10.5194/amt-18-2701-2025, https://doi.org/10.5194/amt-18-2701-2025, 2025
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This study presents high-precision measurements of ∆′17O(CO2). Key findings include the extension of the N2O–∆′17O correlation to the upper troposphere and the identification of significant differences in the N2O–∆′17O slope in StratoClim samples. Additionally, the ∆′17O measurements are used to estimate global stratospheric production and surface removal of ∆′17O, providing an independent estimate of global vegetation CO2 exchange.
Johann Rasmus Nüß, Nikos Daskalakis, Fabian Günther Piwowarczyk, Angelos Gkouvousis, Oliver Schneising, Michael Buchwitz, Maria Kanakidou, Maarten C. Krol, and Mihalis Vrekoussis
Geosci. Model Dev., 18, 2861–2890, https://doi.org/10.5194/gmd-18-2861-2025, https://doi.org/10.5194/gmd-18-2861-2025, 2025
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We estimate carbon monoxide emissions through inverse modeling, an approach where measurements of tracers in the atmosphere are fed to 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.
Juliëtte C. S. Anema, K. Folkert Boersma, Lieuwe G. Tilstra, Olaf N. E. Tuinder, and Willem W. Verstraeten
Atmos. Meas. Tech., 18, 1961–1979, https://doi.org/10.5194/amt-18-1961-2025, https://doi.org/10.5194/amt-18-1961-2025, 2025
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Long-term records of plant fluorescence offer vital insights into changing vegetation activity. The GOME-2A sensor provides extensive global observations but suffers from calibration and instrument degradation, which affects data consistency. This study presents the SIFTER v3 algorithm, which effectively resolves these issues and includes other improvements, resulting in robust, accurate, and consistent GOME-2A fluorescence measurements from 2007 to 2017.
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.
Isolde Glissenaar, Klaas Folkert Boersma, Isidora Anglou, Pieter Rijsdijk, Tijl Verhoelst, Steven Compernolle, Gaia Pinardi, Jean-Christopher Lambert, Michel Van Roozendael, and Henk Eskes
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2024-616, https://doi.org/10.5194/essd-2024-616, 2025
Revised manuscript accepted for ESSD
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We developed a new global dataset of nitrogen dioxide (NO2) levels in the lower atmosphere, using data from TROPOMI for 2018–2021. This dataset offers improved accuracy and detail compared to earlier versions, meeting high international standards for climate data. By refining how measurement errors are calculated and reduced over time and space, we provide clearer insights into pollution patterns. This work supports better air quality monitoring and informs actions to address pollution globally.
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.
Felipe Cifuentes, Henk Eskes, Enrico Dammers, Charlotte Bryan, and Folkert Boersma
Geosci. Model Dev., 18, 621–649, https://doi.org/10.5194/gmd-18-621-2025, https://doi.org/10.5194/gmd-18-621-2025, 2025
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We tested the capability of the flux divergence approach (FDA) to reproduce known NOx emissions using synthetic NO2 satellite column retrievals from high-resolution model simulations. The FDA accurately reproduced NOx emissions when column observations were limited to the boundary layer and when the variability of the NO2 lifetime, the NOx : NO2 ratio, and NO2 profile shapes were correctly modeled. This introduces strong model dependency, reducing the simplicity of the original FDA formulation.
Pieter Rijsdijk, Henk Eskes, Arlene Dingemans, K. Folkert Boersma, Takashi Sekiya, Kazuyuki Miyazaki, and Sander Houweling
Geosci. Model Dev., 18, 483–509, https://doi.org/10.5194/gmd-18-483-2025, https://doi.org/10.5194/gmd-18-483-2025, 2025
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Clustering high-resolution satellite observations into superobservations improves model validation and data assimilation applications. In our paper, we derive quantitative uncertainties for satellite NO2 column observations based on knowledge of the retrievals, including a detailed analysis of spatial error correlations and representativity errors. The superobservations and uncertainty estimates are tested in a global chemical data assimilation system and are found to improve the forecasts.
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.
Mirjam Tijhuis, Bart J. H. van Stratum, and Chiel C. van Heerwaarden
Atmos. Chem. Phys., 24, 10567–10582, https://doi.org/10.5194/acp-24-10567-2024, https://doi.org/10.5194/acp-24-10567-2024, 2024
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Radiative transfer in the atmosphere is a 3D processes, which is often modelled in 1D for computational efficiency. We studied the differences between using 1D and 3D radiative transfer. With 3D radiation, larger clouds that contain more liquid water develop. However, they cover roughly the same part of the sky, and the average total radiation at the surface is nearly unchanged. The increase in cloud size might be important for weather models, as it can impact the formation of rain, for example.
Tong Sha, Siyu Yang, Qingcai Chen, Liangqing Li, Xiaoyan Ma, Yan-Lin Zhang, Zhaozhong Feng, K. Folkert Boersma, and Jun Wang
Atmos. Chem. Phys., 24, 8441–8455, https://doi.org/10.5194/acp-24-8441-2024, https://doi.org/10.5194/acp-24-8441-2024, 2024
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Using an updated soil reactive nitrogen emission scheme in the Unified Inputs for Weather Research and Forecasting coupled with Chemistry (UI-WRF-Chem) model, we investigate the role of soil NO and HONO (Nr) emissions in air quality and temperature in North China. Contributions of soil Nr emissions to O3 and secondary pollutants are revealed, exceeding effects of soil NOx or HONO emission. Soil Nr emissions play an important role in mitigating O3 pollution and addressing climate change.
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.
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.
Juliëtte C. S. Anema, Klaas Folkert Boersma, Piet Stammes, Gerbrand Koren, William Woodgate, Philipp Köhler, Christian Frankenberg, and Jacqui Stol
Biogeosciences, 21, 2297–2311, https://doi.org/10.5194/bg-21-2297-2024, https://doi.org/10.5194/bg-21-2297-2024, 2024
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To keep the Paris agreement goals within reach, negative emissions are necessary. They can be achieved with mitigation techniques, such as reforestation, which remove CO2 from the atmosphere. While governments have pinned their hopes on them, there is not yet a good set of tools to objectively determine whether negative emissions do what they promise. Here we show how satellite measurements of plant fluorescence are useful in detecting carbon uptake due to reforestation and vegetation regrowth.
Tobias Christoph Valentin Werner Riess, Klaas Folkert Boersma, Ward Van Roy, Jos de Laat, Enrico Dammers, and Jasper van Vliet
Atmos. Meas. Tech., 16, 5287–5304, https://doi.org/10.5194/amt-16-5287-2023, https://doi.org/10.5194/amt-16-5287-2023, 2023
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Satellite retrievals of trace gases require prior knowledge of the vertical distribution of the pollutant, which is usually obtained from models. Using aircraft-measured vertical NO2 profiles over the North Sea in summer 2021, we evaluate the Transport Model 5 profiles used in the TROPOMI NO2 retrieval. We conclude that driven by the low horizontal resolution and the overestimated vertical mixing, resulting NO2 columns are 20 % too low. This has important implications for emission estimates.
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.
John Douros, Henk Eskes, Jos van Geffen, K. Folkert Boersma, Steven Compernolle, Gaia Pinardi, Anne-Marlene Blechschmidt, Vincent-Henri Peuch, Augustin Colette, and Pepijn Veefkind
Geosci. Model Dev., 16, 509–534, https://doi.org/10.5194/gmd-16-509-2023, https://doi.org/10.5194/gmd-16-509-2023, 2023
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We focus on the challenges associated with comparing atmospheric composition models with satellite products such as tropospheric NO2 columns. The aim is to highlight the methodological difficulties and propose sound ways of doing such comparisons. Building on the comparisons, a new satellite product is proposed and made available, which takes advantage of higher-resolution, regional atmospheric modelling to improve estimates of troposheric NO2 columns over Europe.
Viral Shah, Daniel J. Jacob, Ruijun Dang, Lok N. Lamsal, Sarah A. Strode, Stephen D. Steenrod, K. Folkert Boersma, Sebastian D. Eastham, Thibaud M. Fritz, Chelsea Thompson, Jeff Peischl, Ilann Bourgeois, Ilana B. Pollack, Benjamin A. Nault, Ronald C. Cohen, Pedro Campuzano-Jost, Jose L. Jimenez, Simone T. Andersen, Lucy J. Carpenter, Tomás Sherwen, and Mat J. Evans
Atmos. Chem. Phys., 23, 1227–1257, https://doi.org/10.5194/acp-23-1227-2023, https://doi.org/10.5194/acp-23-1227-2023, 2023
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NOx in the free troposphere (above 2 km) affects global tropospheric chemistry and the retrieval and interpretation of satellite NO2 measurements. We evaluate free tropospheric NOx in global atmospheric chemistry models and find that recycling NOx from its reservoirs over the oceans is faster than that simulated in the models, resulting in increases in simulated tropospheric ozone and OH. Over the U.S., free tropospheric NO2 contributes the majority of the tropospheric NO2 column in summer.
Qianqian Zhang, K. Folkert Boersma, Bin Zhao, Henk Eskes, Cuihong Chen, Haotian Zheng, and Xingying Zhang
Atmos. Chem. Phys., 23, 551–563, https://doi.org/10.5194/acp-23-551-2023, https://doi.org/10.5194/acp-23-551-2023, 2023
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We developed an improved superposition column model and used the latest released (v2.3.1) TROPOMI satellite NO2 observations to estimate daily city-scale NOx and CO2 emissions. The results are verified against bottom-up emissions and OCO-2 XCO2 observations. We obtained the day-to-day variation of city NOx and CO2 emissions, allowing policymakers to gain real-time information on spatial–temporal emission patterns and the effectiveness of carbon and nitrogen regulation in urban environments.
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.
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.
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.
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.
Jos van Geffen, Henk Eskes, Steven Compernolle, Gaia Pinardi, Tijl Verhoelst, Jean-Christopher Lambert, Maarten Sneep, Mark ter Linden, Antje Ludewig, K. Folkert Boersma, and J. Pepijn Veefkind
Atmos. Meas. Tech., 15, 2037–2060, https://doi.org/10.5194/amt-15-2037-2022, https://doi.org/10.5194/amt-15-2037-2022, 2022
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Nitrogen dioxide (NO2) is one of the main data products measured by the Tropospheric Monitoring Instrument (TROPOMI) on the Sentinel-5 Precursor (S5P) satellite. This study describes improvements in the TROPOMI NO2 retrieval leading to version v2.2, operational since 1 July 2021. It compares results with previous versions v1.2–v1.4 and with Ozone Monitoring Instrument (OMI) and ground-based measurements.
Tobias Christoph Valentin Werner Riess, Klaas Folkert Boersma, Jasper van Vliet, Wouter Peters, Maarten Sneep, Henk Eskes, and Jos van Geffen
Atmos. Meas. Tech., 15, 1415–1438, https://doi.org/10.5194/amt-15-1415-2022, https://doi.org/10.5194/amt-15-1415-2022, 2022
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This paper reports on improved monitoring of ship nitrogen oxide emissions by TROPOMI. With its fantastic resolution we can identify lanes of ship nitrogen dioxide (NO2) pollution not detected from space before. The quality of TROPOMI NO2 data over sea is improved further by recent upgrades in cloud retrievals and the use of sun glint scenes. Lastly, we study the impact of COVID-19 on ship NO2 in European seas and compare the found reductions to emission estimates gained from ship-specific data.
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.
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.
Isabelle De Smedt, Gaia Pinardi, Corinne Vigouroux, Steven Compernolle, Alkis Bais, Nuria Benavent, Folkert Boersma, Ka-Lok Chan, Sebastian Donner, Kai-Uwe Eichmann, Pascal Hedelt, François Hendrick, Hitoshi Irie, Vinod Kumar, Jean-Christopher Lambert, Bavo Langerock, Christophe Lerot, Cheng Liu, Diego Loyola, Ankie Piters, Andreas Richter, Claudia Rivera Cárdenas, Fabian Romahn, Robert George Ryan, Vinayak Sinha, Nicolas Theys, Jonas Vlietinck, Thomas Wagner, Ting Wang, Huan Yu, and Michel Van Roozendael
Atmos. Chem. Phys., 21, 12561–12593, https://doi.org/10.5194/acp-21-12561-2021, https://doi.org/10.5194/acp-21-12561-2021, 2021
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This paper assess the performances of the TROPOMI formaldehyde observations compared to its predecessor OMI at different spatial and temporal scales. We also use a global network of MAX-DOAS instruments to validate both satellite datasets for a large range of HCHO columns. The precision obtained with daily TROPOMI observations is comparable to monthly OMI observations. We present clear detection of weak HCHO column enhancements related to shipping emissions in the Indian Ocean.
Jianfeng Li, Yuhang Wang, Ruixiong Zhang, Charles Smeltzer, Andrew Weinheimer, Jay Herman, K. Folkert Boersma, Edward A. Celarier, Russell W. Long, James J. Szykman, Ruben Delgado, Anne M. Thompson, Travis N. Knepp, Lok N. Lamsal, Scott J. Janz, Matthew G. Kowalewski, Xiong Liu, and Caroline R. Nowlan
Atmos. Chem. Phys., 21, 11133–11160, https://doi.org/10.5194/acp-21-11133-2021, https://doi.org/10.5194/acp-21-11133-2021, 2021
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Comprehensive evaluations of simulated diurnal cycles of NO2 and NOy concentrations, vertical profiles, and tropospheric vertical column densities at two different resolutions with various measurements during the DISCOVER-AQ 2011 campaign show potential distribution biases of NOx emissions in the National Emissions Inventory 2011 at both 36 and 4 km resolutions, providing another possible explanation for the overestimation of model results.
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).
Anteneh Getachew Mengistu, Gizaw Mengistu Tsidu, Gerbrand Koren, Maurits L. Kooreman, K. Folkert Boersma, Torbern Tagesson, Jonas Ardö, Yann Nouvellon, and Wouter Peters
Biogeosciences, 18, 2843–2857, https://doi.org/10.5194/bg-18-2843-2021, https://doi.org/10.5194/bg-18-2843-2021, 2021
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In this study, we assess the usefulness of Sun-Induced Fluorescence of Terrestrial Ecosystems Retrieval (SIFTER) data from the GOME-2A instrument and near-infrared reflectance of vegetation (NIRv) from MODIS to capture the seasonality and magnitudes of gross primary production (GPP) derived from six eddy-covariance flux towers in Africa in the overlap years between 2007–2014. We also test the robustness of sun-induced fluoresence and NIRv to compare the seasonality of GPP for the major biomes.
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.
Eloise A. Marais, John F. Roberts, Robert G. Ryan, Henk Eskes, K. Folkert Boersma, Sungyeon Choi, Joanna Joiner, Nader Abuhassan, Alberto Redondas, Michel Grutter, Alexander Cede, Laura Gomez, and Monica Navarro-Comas
Atmos. Meas. Tech., 14, 2389–2408, https://doi.org/10.5194/amt-14-2389-2021, https://doi.org/10.5194/amt-14-2389-2021, 2021
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Nitrogen oxides in the upper troposphere have a profound influence on the global troposphere, but routine reliable observations there are exceedingly rare. We apply cloud-slicing to TROPOMI total columns of nitrogen dioxide (NO2) at high spatial resolution to derive near-global observations of NO2 in the upper troposphere and show consistency with existing datasets. These data offer tremendous potential to address knowledge gaps in this oft underappreciated portion of the atmosphere.
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.
Tijl Verhoelst, Steven Compernolle, Gaia Pinardi, Jean-Christopher Lambert, Henk J. Eskes, Kai-Uwe Eichmann, Ann Mari Fjæraa, José Granville, Sander Niemeijer, Alexander Cede, Martin Tiefengraber, François Hendrick, Andrea Pazmiño, Alkiviadis Bais, Ariane Bazureau, K. Folkert Boersma, Kristof Bognar, Angelika Dehn, Sebastian Donner, Aleksandr Elokhov, Manuel Gebetsberger, Florence Goutail, Michel Grutter de la Mora, Aleksandr Gruzdev, Myrto Gratsea, Georg H. Hansen, Hitoshi Irie, Nis Jepsen, Yugo Kanaya, Dimitris Karagkiozidis, Rigel Kivi, Karin Kreher, Pieternel F. Levelt, Cheng Liu, Moritz Müller, Monica Navarro Comas, Ankie J. M. Piters, Jean-Pierre Pommereau, Thierry Portafaix, Cristina Prados-Roman, Olga Puentedura, Richard Querel, Julia Remmers, Andreas Richter, John Rimmer, Claudia Rivera Cárdenas, Lidia Saavedra de Miguel, Valery P. Sinyakov, Wolfgang Stremme, Kimberly Strong, Michel Van Roozendael, J. Pepijn Veefkind, Thomas Wagner, Folkard Wittrock, Margarita Yela González, and Claus Zehner
Atmos. Meas. Tech., 14, 481–510, https://doi.org/10.5194/amt-14-481-2021, https://doi.org/10.5194/amt-14-481-2021, 2021
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This paper reports on the ground-based validation of the NO2 data produced operationally by the TROPOMI instrument on board the Sentinel-5 Precursor satellite. Tropospheric, stratospheric, and total NO2 columns are compared to measurements collected from MAX-DOAS, ZSL-DOAS, and PGN/Pandora instruments respectively. The products are found to satisfy mission requirements in general, though negative mean differences are found at sites with high pollution levels. Potential causes are discussed.
Gaia Pinardi, Michel Van Roozendael, François Hendrick, Nicolas Theys, Nader Abuhassan, Alkiviadis Bais, Folkert Boersma, Alexander Cede, Jihyo Chong, Sebastian Donner, Theano Drosoglou, Anatoly Dzhola, Henk Eskes, Udo Frieß, José Granville, Jay R. Herman, Robert Holla, Jari Hovila, Hitoshi Irie, Yugo Kanaya, Dimitris Karagkiozidis, Natalia Kouremeti, Jean-Christopher Lambert, Jianzhong Ma, Enno Peters, Ankie Piters, Oleg Postylyakov, Andreas Richter, Julia Remmers, Hisahiro Takashima, Martin Tiefengraber, Pieter Valks, Tim Vlemmix, Thomas Wagner, and Folkard Wittrock
Atmos. Meas. Tech., 13, 6141–6174, https://doi.org/10.5194/amt-13-6141-2020, https://doi.org/10.5194/amt-13-6141-2020, 2020
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We validate several GOME-2 and OMI tropospheric NO2 products with 23 MAX-DOAS and 16 direct sun instruments distributed worldwide, highlighting large horizontal inhomogeneities at several sites affecting the validation results. We propose a method for quantification and correction. We show the application of such correction reduces the satellite underestimation in almost all heterogeneous cases, but a negative bias remains over the MAX-DOAS and direct sun network ensemble for both satellites.
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.
Kazuyuki Miyazaki, Kevin Bowman, Takashi Sekiya, Henk Eskes, Folkert Boersma, Helen Worden, Nathaniel Livesey, Vivienne H. Payne, Kengo Sudo, Yugo Kanaya, Masayuki Takigawa, and Koji Ogochi
Earth Syst. Sci. Data, 12, 2223–2259, https://doi.org/10.5194/essd-12-2223-2020, https://doi.org/10.5194/essd-12-2223-2020, 2020
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This study presents the results from the Tropospheric Chemistry Reanalysis version 2 (TCR-2) for 2005–2018 obtained from the assimilation of multiple satellite measurements of ozone, CO, NO2, HNO3, and SO2 from the OMI, SCIAMACHY, GOME-2, TES, MLS, and MOPITT instruments. The evaluation results demonstrate the capability of the reanalysis products to improve understanding of the processes controlling variations in atmospheric composition, including long-term changes in air quality and emissions.
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Short summary
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.
This paper presents detailed plume simulations of nitrogen oxides and carbon dioxide that are...
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