Articles | Volume 25, issue 14
https://doi.org/10.5194/acp-25-7925-2025
© Author(s) 2025. 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-25-7925-2025
© Author(s) 2025. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
25 Jul 2025
Research article |
| 25 Jul 2025
| 25 Jul 2025
Characterization of reactive oxidized nitrogen in the global upper troposphere using recent and historic commercial and research aircraft campaigns and GEOS-Chem
Department of Geography, University College London, London, UK
Department of Geography, University College London, London, UK
Gongda Lu
Department of Geography, University College London, London, UK
now at: the Satellite Application Center for Ecology and Environment, Ministry of Ecology and Environment, Beijing, China
Robert G. Ryan
Department of Geography, University College London, London, UK
now at: School of Geography, Earth and Atmospheric Science, University of Melbourne, Melbourne, Australia
Bastien Sauvage
Laboratoire d'Aérologie, Université de Toulouse, CNRS, Université Toulouse III Paul Sabatier, Toulouse, France
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Rebekah P. Horner, Eloise A. Marais, Nana Wei, Robert G. Ryan, and Viral Shah
Atmos. Chem. Phys., 24, 13047–13064, https://doi.org/10.5194/acp-24-13047-2024, https://doi.org/10.5194/acp-24-13047-2024, 2024
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Nitrogen oxides (NOx ≡ NO + NO2) affect tropospheric ozone and the hydroxyl radical, influencing climate and atmospheric oxidation. To address the lack of routine observations of NOx, we cloud slice satellite observations of NO2 to derive a new dataset of global vertical profiles of NO2. We evaluate our data against in situ aircraft observations and use these data to critique the contemporary understanding of tropospheric NOx, as simulated by the GEOS-Chem model.
William J. Collins, Fiona M. O'Connor, Rachael E. Byrom, Øivind Hodnebrog, Patrick Jöckel, Mariano Mertens, Gunnar Myhre, Matthias Nützel, Dirk Olivié, Ragnhild Bieltvedt Skeie, Laura Stecher, Larry W. Horowitz, Vaishali Naik, Gregory Faluvegi, Ulas Im, Lee T. Murray, Drew Shindell, Kostas Tsigaridis, Nathan Luke Abraham, and James Keeble
Atmos. Chem. Phys., 25, 9031–9060, https://doi.org/10.5194/acp-25-9031-2025, https://doi.org/10.5194/acp-25-9031-2025, 2025
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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
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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.
Anne M. Thompson, Ryan M. Stauffer, Debra E. Kollonige, Jerald R. Ziemke, Maria Cazorla, Pawel Wolff, and Bastien Sauvage
EGUsphere, https://doi.org/10.5194/egusphere-2024-3761, https://doi.org/10.5194/egusphere-2024-3761, 2025
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This paper uses tropical ozone profiles from balloon borne instruments and aircraft to show that ozone in the free troposphere is not growing fast except over equatorial SE Asia.
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EGUsphere, https://doi.org/10.5194/egusphere-2024-3748, https://doi.org/10.5194/egusphere-2024-3748, 2025
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Tropospheric ozone is a potent greenhouse gas; its anthropogenic levels rise contributes to climate change. We evaluate tropospheric ozone trends and climate impacts with aircraft data and a radiative model, comparing the baseline period (1994–2004) to 2011–2016 and 2019. Tropospheric ozone levels increased significantly but with a smaller trend in 2019 than in 2011–2016. However, ozone radiative forcing did not decrease between these periods because of different vertical distribution evolutions
Eric Martial Yao, Fabien Solmon, Marcellin Adon, Claire Delon, Corinne Galy-Lacaux, Graziano Giuliani, Bastien Sauvage, and Véronique Yoboue
EGUsphere, https://doi.org/10.5194/egusphere-2024-3179, https://doi.org/10.5194/egusphere-2024-3179, 2025
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As climate change and human activities intensify in Africa, understanding how air pollution, climate, and natural cycles interact is crucial. This study explores how nitrogen oxide emissions from African soils, especially in dry regions, contribute to atmospheric pollution. By using a climate-chemistry model, we show that considering these emissions improves predictions of nitrogen dioxide, nitric acid and ozone, although some discrepancies remain compared to observations.
Brice Barret, Pierre Loicq, Eric Le Flochmoën, Yasmine Bennouna, Juliette Hadji-Lazaro, Daniel Hurtmans, and Bastien Sauvage
Atmos. Meas. Tech., 18, 129–149, https://doi.org/10.5194/amt-18-129-2025, https://doi.org/10.5194/amt-18-129-2025, 2025
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Profiles of carbon monoxide (CO) retrieved from the Infrared Atmospheric Sounding Interferometer (IASI) with the SOftware for a Fast Retrieval of IASI Data (SOFRID) and Fast Optimal Retrievals on Layers for IASI (FORLI) are validated with 8500 observations at 33 airports from the In-service Aircraft for a Global Observing System (IAGOS) for 2008–2019. IASI retrievals underestimate CO, with stronger bias in the middle to upper troposphere for SOFRID and in the lower troposphere for FORLI.
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.
Rebekah P. Horner, Eloise A. Marais, Nana Wei, Robert G. Ryan, and Viral Shah
Atmos. Chem. Phys., 24, 13047–13064, https://doi.org/10.5194/acp-24-13047-2024, https://doi.org/10.5194/acp-24-13047-2024, 2024
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Nitrogen oxides (NOx ≡ NO + NO2) affect tropospheric ozone and the hydroxyl radical, influencing climate and atmospheric oxidation. To address the lack of routine observations of NOx, we cloud slice satellite observations of NO2 to derive a new dataset of global vertical profiles of NO2. We evaluate our data against in situ aircraft observations and use these data to critique the contemporary understanding of tropospheric NOx, as simulated by the GEOS-Chem model.
Audrey Gaudel, Ilann Bourgeois, Meng Li, Kai-Lan Chang, Jerald Ziemke, Bastien Sauvage, Ryan M. Stauffer, Anne M. Thompson, Debra E. Kollonige, Nadia Smith, Daan Hubert, Arno Keppens, Juan Cuesta, Klaus-Peter Heue, Pepijn Veefkind, Kenneth Aikin, Jeff Peischl, Chelsea R. Thompson, Thomas B. Ryerson, Gregory J. Frost, Brian C. McDonald, and Owen R. Cooper
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Robert G. Ryan, Eloise A. Marais, Eleanor Gershenson-Smith, Robbie Ramsay, Jan-Peter Muller, Jan-Lukas Tirpitz, and Udo Frieß
Atmos. Chem. Phys., 23, 7121–7139, https://doi.org/10.5194/acp-23-7121-2023, https://doi.org/10.5194/acp-23-7121-2023, 2023
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Haolin Wang, Xiao Lu, Daniel J. Jacob, Owen R. Cooper, Kai-Lan Chang, Ke Li, Meng Gao, Yiming Liu, Bosi Sheng, Kai Wu, Tongwen Wu, Jie Zhang, Bastien Sauvage, Philippe Nédélec, Romain Blot, and Shaojia Fan
Atmos. Chem. Phys., 22, 13753–13782, https://doi.org/10.5194/acp-22-13753-2022, https://doi.org/10.5194/acp-22-13753-2022, 2022
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We report significant global tropospheric ozone increases in 1995–2017 based on extensive aircraft and ozonesonde observations. Using GEOS-Chem (Goddard Earth Observing System chemistry model) multi-decadal global simulations, we find that changes in global anthropogenic emissions, in particular the rapid increases in aircraft emissions, contribute significantly to the increases in tropospheric ozone and resulting radiative impact.
Andrea Mazzeo, Michael Burrow, Andrew Quinn, Eloise A. Marais, Ajit Singh, David Ng'ang'a, Michael J. Gatari, and Francis D. Pope
Atmos. Chem. Phys., 22, 10677–10701, https://doi.org/10.5194/acp-22-10677-2022, https://doi.org/10.5194/acp-22-10677-2022, 2022
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A modelling system for meteorology and chemistry transport processes, WRF–CHIMERE, has been tested and validated for three East African conurbations using the most up-to-date anthropogenic emissions available. Results show that the model is able to reproduce hourly and daily temporal variabilities in aerosol concentrations that are close to observations in both urban and rural environments, encouraging the adoption of numerical modelling as a tool for air quality management in East Africa.
Marios Panagi, Roberto Sommariva, Zoë L. Fleming, Paul S. Monks, Gongda Lu, Eloise A. Marais, James R. Hopkins, Alastair C. Lewis, Qiang Zhang, James D. Lee, Freya A. Squires, Lisa K. Whalley, Eloise J. Slater, Dwayne E. Heard, Robert Woodward-Massey, Chunxiang Ye, and Joshua D. Vande Hey
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-379, https://doi.org/10.5194/acp-2022-379, 2022
Revised manuscript not accepted
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A dispersion model and a box model were combined to investigate the evolution of VOCs in Beijing once they are emitted from anthropogenic sources. It was determined that during the winter time the VOC concentrations in Beijing are driven predominantly by sources within Beijing and by a combination of transport and chemistry during the summer. Furthermore, the results in the paper highlight the need for a season specific policy.
Richard J. Pope, Rebecca Kelly, Eloise A. Marais, Ailish M. Graham, Chris Wilson, Jeremy J. Harrison, Savio J. A. Moniz, Mohamed Ghalaieny, Steve R. Arnold, and Martyn P. Chipperfield
Atmos. Chem. Phys., 22, 4323–4338, https://doi.org/10.5194/acp-22-4323-2022, https://doi.org/10.5194/acp-22-4323-2022, 2022
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Nitrogen oxides (NOx) are potent air pollutants which directly impact on human health. In this study, we use satellite nitrogen dioxide (NO2) data to evaluate the spatial distribution and temporal evolution of the UK official NOx emissions inventory, with reasonable agreement. We also derived satellite-based NOx emissions for several UK cities. In the case of London and Birmingham, the NAEI NOx emissions are potentially too low by >50%.
Graciela B. Raga, Darrel Baumgardner, Blanca Rios, Yanet Díaz-Esteban, Alejandro Jaramillo, Martin Gallagher, Bastien Sauvage, Pawel Wolff, and Gary Lloyd
Atmos. Chem. Phys., 22, 2269–2292, https://doi.org/10.5194/acp-22-2269-2022, https://doi.org/10.5194/acp-22-2269-2022, 2022
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The In-Service Aircraft for a Global Observing System (IAGOS) is a small fleet of commercial aircraft that carry a suite of meteorological, gas, aerosol, and cloud sensors and have been measuring worldwide for almost 9 years, since late 2011. Extreme ice events (EIEs) have been identified from the IAGOS cloud measurements and linked to surface emissions for biomass and fossil fuel consumption. The results reported here are highly relevant for climate change and flight operations forecasting.
Hannah Clark, Yasmine Bennouna, Maria Tsivlidou, Pawel Wolff, Bastien Sauvage, Brice Barret, Eric Le Flochmoën, Romain Blot, Damien Boulanger, Jean-Marc Cousin, Philippe Nédélec, Andreas Petzold, and Valérie Thouret
Atmos. Chem. Phys., 21, 16237–16256, https://doi.org/10.5194/acp-21-16237-2021, https://doi.org/10.5194/acp-21-16237-2021, 2021
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We examined 27 years of IAGOS (In-service Aircraft for a Global Observing System) profiles at Frankfurt to see if there were unusual features during the spring of 2020 related to COVID-19 lockdowns in Europe. Increased ozone near the surface was partly linked to the reduction in emissions. Carbon monoxide decreased near the surface, but the impact of the lockdowns was offset by polluted air masses from elsewhere. There were small reductions in ozone and carbon monoxide in the free troposphere.
Victor Lannuque, Bastien Sauvage, Brice Barret, Hannah Clark, Gilles Athier, Damien Boulanger, Jean-Pierre Cammas, Jean-Marc Cousin, Alain Fontaine, Eric Le Flochmoën, Philippe Nédélec, Hervé Petetin, Isabelle Pfaffenzeller, Susanne Rohs, Herman G. J. Smit, Pawel Wolff, and Valérie Thouret
Atmos. Chem. Phys., 21, 14535–14555, https://doi.org/10.5194/acp-21-14535-2021, https://doi.org/10.5194/acp-21-14535-2021, 2021
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The African intertropical troposphere is one of the world areas where the increase in ozone mixing ratio has been most pronounced since 1980 and where high carbon monoxide mixing ratios are found in altitude. In this article, IAGOS aircraft measurements, IASI satellite instrument observations, and SOFT-IO model products are used to explore the seasonal distribution variations and the origin of ozone and carbon monoxide over the African upper troposphere.
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.
Gongda Lu, Eloise A. Marais, Tuan V. Vu, Jingsha Xu, Zongbo Shi, James D. Lee, Qiang Zhang, Lu Shen, Gan Luo, and Fangqun Yu
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-428, https://doi.org/10.5194/acp-2021-428, 2021
Revised manuscript not accepted
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Emission controls were imposed in Beijing-Tianjin-Hebei in northern China in autumn-winter 2017. We find that regional PM2.5 targets (15 % decrease relative to previous year) were exceeded. Our analysis shows that decline in precursor emissions only leads to less than half (43 %) the improved air quality. Most of the change (57 %) is due to interannual variability in meteorology. Stricter emission controls may be necessary in years with unfavourable meteorology.
Romain Blot, Philippe Nedelec, Damien Boulanger, Pawel Wolff, Bastien Sauvage, Jean-Marc Cousin, Gilles Athier, Andreas Zahn, Florian Obersteiner, Dieter Scharffe, Hervé Petetin, Yasmine Bennouna, Hannah Clark, and Valérie Thouret
Atmos. Meas. Tech., 14, 3935–3951, https://doi.org/10.5194/amt-14-3935-2021, https://doi.org/10.5194/amt-14-3935-2021, 2021
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A lack of information about temporal changes in measurement uncertainties is an area of concern for long-term trend studies of the key compounds which have a direct or indirect impact on climate change. The IAGOS program has measured O3 and CO within the troposphere and lower stratosphere for more than 25 years. In this study, we demonstrated that the IAGOS database can be treated as one continuous program and is therefore appropriate for studies of long-term trends.
Karn Vohra, Eloise A. Marais, Shannen Suckra, Louisa Kramer, William J. Bloss, Ravi Sahu, Abhishek Gaur, Sachchida N. Tripathi, Martin Van Damme, Lieven Clarisse, and Pierre-F. Coheur
Atmos. Chem. Phys., 21, 6275–6296, https://doi.org/10.5194/acp-21-6275-2021, https://doi.org/10.5194/acp-21-6275-2021, 2021
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We find satellite observations of atmospheric composition generally reproduce variability in surface air pollution, so we use their long record to estimate air quality trends in major UK and Indian cities. Our trend analysis shows that pollutants targeted with air quality policies have not declined in Delhi and Kanpur but have in London and Birmingham, with the exception of a recent and dramatic increase in reactive volatile organics in London. Unregulated ammonia has increased only in Delhi.
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.
Christoph A. Keller, Mathew J. Evans, K. Emma Knowland, Christa A. Hasenkopf, Sruti Modekurty, Robert A. Lucchesi, Tomohiro Oda, Bruno B. Franca, Felipe C. Mandarino, M. Valeria Díaz Suárez, Robert G. Ryan, Luke H. Fakes, and Steven Pawson
Atmos. Chem. Phys., 21, 3555–3592, https://doi.org/10.5194/acp-21-3555-2021, https://doi.org/10.5194/acp-21-3555-2021, 2021
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This study combines surface observations and model simulations to quantify the impact of COVID-19 restrictions on air quality across the world. The presented methodology removes the confounding impacts of meteorology on air pollution. Our results indicate that surface concentrations of nitrogen dioxide, an important air pollutant emitted during the combustion of fossil fuels, declined by up to 60 % following the implementation of COVID-19 containment measures.
Keun-Ok Lee, Brice Barret, Eric L. Flochmoën, Pierre Tulet, Silvia Bucci, Marc von Hobe, Corinna Kloss, Bernard Legras, Maud Leriche, Bastien Sauvage, Fabrizio Ravegnani, and Alexey Ulanovsky
Atmos. Chem. Phys., 21, 3255–3274, https://doi.org/10.5194/acp-21-3255-2021, https://doi.org/10.5194/acp-21-3255-2021, 2021
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This paper focuses on the emission sources and pathways of pollution from the boundary layer to the Asian monsoon anticyclone (AMA) during the StratoClim aircraft campaign period. Simulations with the Meso-NH cloud-chemistry model at a horizontal resolution of 15 km are performed over the Asian region to characterize the impact of monsoon deep convection on the composition of AMA and on the formation of the Asian tropopause aerosol layer during the StratoClim campaign.
Robert G. Ryan, Jeremy D. Silver, Richard Querel, Dan Smale, Steve Rhodes, Matt Tully, Nicholas Jones, and Robyn Schofield
Atmos. Meas. Tech., 13, 6501–6519, https://doi.org/10.5194/amt-13-6501-2020, https://doi.org/10.5194/amt-13-6501-2020, 2020
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Models have identified Australasia as a formaldehyde (HCHO) hotspot from vegetation sources, but few measurement studies exist to verify this. We compare, and find good agreement between, HCHO measurements using three – two ground-based and one satellite-based – different spectroscopic techniques in Australia and New Zealand. This gives confidence in using satellite observations to study HCHO and associated air chemistry and pollution problems in this under-studied part of the world.
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Short summary
This study uses reactive nitrogen observations from NASA DC-8 research aircraft and the In-service Aircraft for a Global Observing System (IAGOS) campaigns to characterize reactive nitrogen seasonality and composition in the global upper troposphere and to diagnose the greatest knowledge gaps from comparison to a state-of-the-science model, GEOS-Chem, that need to be resolved for climate, nitrogen cycle, and air pollution assessments.
This study uses reactive nitrogen observations from NASA DC-8 research aircraft and the...
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