Articles | Volume 24, issue 24
https://doi.org/10.5194/acp-24-13913-2024
© 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-24-13913-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
16 Dec 2024
Research article |
| 16 Dec 2024
| 16 Dec 2024
The potential of drone observations to improve air quality predictions by 4D-Var
Hassnae Erraji
Forschungszentrum Jülich GmbH, Institute of Climate and Energy Systems – Troposphere (ICE-3), Jülich, Germany
Philipp Franke
Forschungszentrum Jülich GmbH, Institute of Climate and Energy Systems – Troposphere (ICE-3), Jülich, Germany
Astrid Lampert
Institute of Flight Guidance, TU Braunschweig, Braunschweig, Germany
Tobias Schuldt
Forschungszentrum Jülich GmbH, Institute of Climate and Energy Systems – Troposphere (ICE-3), Jülich, Germany
Ralf Tillmann
Forschungszentrum Jülich GmbH, Institute of Climate and Energy Systems – Troposphere (ICE-3), Jülich, Germany
Andreas Wahner
Forschungszentrum Jülich GmbH, Institute of Climate and Energy Systems – Troposphere (ICE-3), Jülich, Germany
Anne Caroline Lange
CORRESPONDING AUTHOR
Forschungszentrum Jülich GmbH, Institute of Climate and Energy Systems – Troposphere (ICE-3), Jülich, Germany
Related authors
No articles found.
Astrid Lampert, Beatriz Cañadillas, Thomas Rausch, Lea Schmitt, Bughsin' Djath, Johannes Schulz-Stellenfleth, Andreas Platis, Kjell zum Berge, Ines Schäfer, Jens Bange, Thomas Neumann, Martin Dörenkämper, Bernhard Stoevesandt, Julia Gottschall, Lukas Vollmer, Stefan Emeis, Mares Barekzai, Simon Siedersleben, Martin Kühn, Gerald Steinfeld, Detlev Heinemann, Joachim Peinke, Hendrik Heißelmann, Jörge Schneemann, Gabriele Centurelli, Philipp Waldmann, and Konrad Bärfuss
Wind Energ. Sci. Discuss., https://doi.org/10.5194/wes-2025-277, https://doi.org/10.5194/wes-2025-277, 2026
Preprint under review for WES
Short summary
Short summary
Two major aircraft measurement campaigns above the North Sea provide insights into modifications of the wind field and sea surface induced by wind farms: The aircraft performed transects at hub height upstream and downstream of wind farm clusters, and identified different effects, e.g., how long it takes for the wind speed to recover after the wind farm, how changes across the coastline interact with wind energy, and if wind farms are well represented in numerical simulations.
Yuwei Wang, Aristeidis Voliotis, Emily Matthews, Rongrong Wu, Milan Roska, Max Gerrit Adam, René Dubus, Lukas Kesper, Franz Rohrer, Robert Wegener, Benjamin Winter, Kelvin H. Bates, Quanfu He, Thorsten Hohaus, Achim Grasse, Ralf Tillmann, Andreas Wahner, Hui Wang, Christian Wesolek, Sergej Wedel, Yizhen Wu, Sören R. Zorn, Manjula Canagaratna, Douglas Worsnop, Felipe Lopez-Hilfiker, Georgios I. Gkatzelis, Hugh Coe, and Thomas J. Bannan
EGUsphere, https://doi.org/10.5194/egusphere-2025-6102, https://doi.org/10.5194/egusphere-2025-6102, 2026
This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
Short summary
Short summary
This work developed voltage scanning based calibration approach for a multi-reagent chemical ionization mass spectrometry. This approach improves sensitivity determination for gas-phase compounds. It does not require a calibrant for the target analyte and can estimate sensitivity with acceptable uncertainty based on the experimentally established relationship between binding energies and measured sensitivities. This work is broadly relevant to mass-spectrometric calibration strategies.
Anna Voss, Konrad B. Bärfuss, Beatriz Cañadillas, Maik Angermann, Mark Bitter, Matthias Cremer, Thomas Feuerle, Jonas Spoor, Julie K. Lundquist, Patrick Moriarty, and Astrid Lampert
Wind Energ. Sci., 11, 71–88, https://doi.org/10.5194/wes-11-71-2026, https://doi.org/10.5194/wes-11-71-2026, 2026
Short summary
Short summary
This study analyzes onshore wind farm wakes in a semi-complex terrain with data conducted with the research aircraft of TU Braunschweig during the American WAKE experimeNt (AWAKEN). Vertical profiles of temperature, humidity, and wind give insights into the stratification of the atmospheric boundary layer, while horizontal profiles downwind of wind farms reveal an amplification of the reduction in wind speed in a semi-complex terrain, in particular at a distance of 10 km.
Farhan R. Nursanto, Quanfu He, Sophia van de Wouw, Annika Zanders, Thorsten Hohaus, Willem S. J. Kroese, Robert Wegener, Max Gerrit Adam, Benjamin Winter, René Dubus, Lukas Kesper, Franz Rohrer, Yuwei Wang, Emily Matthews, Aristeidis Voliotis, Thomas J. Bannan, Gordon McFiggans, Hugh Coe, Yizhen Wu, Milan Roska, Manjula Canagaratna, Mitch Alton, Matthew M. Coggon, Chelsea E. Stockwell, Kelvin H. Bates, Eva Y. Pfannerstill, Sören R. Zorn, Hui Wang, Matthieu Riva, Sebastien Perrier, Boxing Yang, Lu Liu, Anna Novelli, Michelle Färber, Hendrik Fuchs, Andrea Carolina Marcillo Lara, Achim Grasse, Christian Wesolek, Ralf Tillmann, Rupert Holzinger, Maarten C. Krol, Georgios I. Gkatzelis, and Juliane L. Fry
EGUsphere, https://doi.org/10.5194/egusphere-2025-6310, https://doi.org/10.5194/egusphere-2025-6310, 2026
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
Short summary
Short summary
Urban air contains reactive gases that can form organic nitrate particles and carry nitrogen oxides pollution far from cities. We recreated urban emissions in a large atmospheric chamber and observed their reactions under day and night conditions. We found that these emissions form organic nitrate particles similar to those from natural sources, with higher amounts and heavier particles at night, making nitrogen pollution longer lived and likely to travel further before depositing on ecosystems.
Amanda Sellmaier, Ellen Damm, Torsten Sachs, Benjamin Kirbus, Inge Wiekenkamp, Annette Rinke, Falk Pätzold, Daiki Nomura, Astrid Lampert, and Markus Rex
Atmos. Chem. Phys., 25, 17685–17700, https://doi.org/10.5194/acp-25-17685-2025, https://doi.org/10.5194/acp-25-17685-2025, 2025
Short summary
Short summary
This study presents continuous ship-borne measurements of methane (CH4) concentration and isotopic composition monitored during an ice drift expedition in 2020. Using trajectory analysis, we linked atmospheric CH4 variabilities to air mass pathways transported over open water or sea-ice. The study highlights the potential of ship-borne observations to fill significant data gaps in the high Arctic.
Alexander Hermanns, Anne Caroline Lange, Julia Kowalski, Hendrik Fuchs, and Philipp Franke
Geosci. Model Dev., 18, 9417–9432, https://doi.org/10.5194/gmd-18-9417-2025, https://doi.org/10.5194/gmd-18-9417-2025, 2025
Short summary
Short summary
For air quality analyses, data assimilation models split available data into assimilation and validation data sets. The former is used to generate the analysis, the latter to verify the simulations. A preprocessor classifying the observations by the data characteristics is developed based on clustering algorithms. The assimilation and validation data sets are compiled by equally allocating data of each cluster. The resulting improvement of the analysis is evaluated with an air quality model.
Eric Förster, Heidi Huntrieser, Michael Lichtenstern, Falk Pätzold, Lutz Bretschneider, Andreas Schlerf, Sven Bollmann, Astrid Lampert, Jarosław Nęcki, Paweł Jagoda, Justyna Swolkień, Dominika Pasternak, Robert A. Field, and Anke Roiger
Atmos. Meas. Tech., 18, 7153–7176, https://doi.org/10.5194/amt-18-7153-2025, https://doi.org/10.5194/amt-18-7153-2025, 2025
Short summary
Short summary
We introduce a helicopter-borne mass balance approach, utilizing the HELiPOD platform, to accurately quantify methane (CH4) emissions from coal mining activities. The comparison of our top-down mass flux estimates (up to 3000 kg h−1) against those from bottom-up in-mine CH4 safety sensors revealed very good agreement. This approach also has a great potential in quantifying emission source strengths (down to 20 kg h−1) from a wide range of other CH4 emitters (e.g. landfills, oil & gas industry).
Lu Liu, Thorsten Hohaus, Andreas Hofzumahaus, Frank Holland, Hendrik Fuchs, Ralf Tillmann, Birger Bohn, Stefanie Andres, Zhaofeng Tan, Franz Rohrer, Vlassis A. Karydis, Vaishali Vardhan, Philipp Franke, Anne C. Lange, Anna Novelli, Benjamin Winter, Changmin Cho, Iulia Gensch, Sergej Wedel, Andreas Wahner, and Astrid Kiendler-Scharr
Atmos. Chem. Phys., 25, 16189–16213, https://doi.org/10.5194/acp-25-16189-2025, https://doi.org/10.5194/acp-25-16189-2025, 2025
Short summary
Short summary
We measured air particles at a rural site in Germany over a year to understand how their sources and properties change with the seasons. Particles from natural sources peaked in summer, especially during heatwaves, while those from burning activities like residential heating and wildfires dominated in colder months. Winds carrying air from other regions also influenced particle levels. These findings link air quality to climate change and energy transitions.
Sungah Kang, Jürgen Wildt, Iida Pullinen, Luc Vereecken, Cheng Wu, Andreas Wahner, Sören R. Zorn, and Thomas F. Mentel
Atmos. Chem. Phys., 25, 15715–15740, https://doi.org/10.5194/acp-25-15715-2025, https://doi.org/10.5194/acp-25-15715-2025, 2025
Short summary
Short summary
Highly oxygenated organic molecules by atmospheric oxidation of plant emitted monoterpenes are important components in secondary organic aerosol formation. Autoxidation of organic peroxy radicals is one important pathway of their formation. We show that isomerization of highly oxygenated alkoxy radicals leads to highly oxygenated peroxy radicals that continue the autoxidation chain. Alkoxy-peroxy steps may dominate the formation of highly oxygenated molecules at high nitrogen oxide levels.
Augustin Colette, Gaëlle Collin, François Besson, Etienne Blot, Vincent Guidard, Frédérik Meleux, Adrien Royer, Valentin Petiot, Claire Miller, Oihana Fermond, Alizé Jeant, Mario Adani, Joaquim Arteta, Anna Benedictow, Robert Bergström, Dene Bowdalo, Jorgen Brandt, Gino Briganti, Ana C. Carvalho, Jesper Heile Christensen, Florian Couvidat, Ilaria D'Elia, Massimo D'Isidoro, Hugo Denier van der Gon, Gaël Descombes, Enza Di Tomaso, John Douros, Jeronimo Escribano, Henk Eskes, Hilde Fagerli, Yalda Fatahi, Johannes Flemming, Elmar Friese, Lise Frohn, Michael Gauss, Camilla Geels, Guido Guarnieri, Marc Guevara, Antoine Guion, Jonathan Guth, Risto Hänninen, Kaj Hansen, Ulas Im, Ruud Janssen, Marine Jeoffrion, Mathieu Joly, Luke Jones, Oriol Jorba, Evgeni Kadantsev, Michael Kahnert, Jacek W. Kaminski, Rostislav Kouznetsov, Richard Kranenburg, Jeroen Kuenen, Anne Caroline Lange, Joachim Langner, Victor Lannuque, Francesca Macchia, Astrid Manders, Mihaela Mircea, Agnes Nyiri, Miriam Olid, Carlos Pérez García-Pando, Yuliia Palamarchuk, Antonio Piersanti, Blandine Raux, Miha Razinger, Lennard Robertson, Arjo Segers, Martijn Schaap, Pilvi Siljamo, David Simpson, Mikhail Sofiev, Anders Stangel, Joanna Struzewska, Carles Tena, Renske Timmermans, Thanos Tsikerdekis, Svetlana Tsyro, Svyatoslav Tyuryakov, Anthony Ung, Andreas Uppstu, Alvaro Valdebenito, Peter van Velthoven, Lina Vitali, Zhuyun Ye, Vincent-Henri Peuch, and Laurence Rouïl
Geosci. Model Dev., 18, 6835–6883, https://doi.org/10.5194/gmd-18-6835-2025, https://doi.org/10.5194/gmd-18-6835-2025, 2025
Short summary
Short summary
The Copernicus Atmosphere Monitoring Service – Regional Production delivers daily forecasts, analyses, and reanalyses of air quality in Europe. The service relies on a distributed modelling production by 11 leading European modelling teams following stringent requirements with an operational design that has no equivalent in the world. All the products are free, open, and quality-assured and disseminated with a high level of reliability.
Alexander Mönnig, Ansgar Hahn, Astrid Lampert, and Ulrich Römer
Wind Energ. Sci. Discuss., https://doi.org/10.5194/wes-2025-112, https://doi.org/10.5194/wes-2025-112, 2025
Revised manuscript not accepted
Short summary
Short summary
To enable efficient load estimation in wind farms, e.g. to assess Remaining Useful Life, we investigated the feasibility of using surrogate models based on open-source turbine models. In a case study, we adapted such a model to match turbines from a real German onshore wind farm, ran aeroelastic simulations, and trained surrogate models to reconstruct loads observed in 5 years of SCADA data. Comparing predicted and measured values showed promising accuracy, especially for blade bending moments.
Michael Rolletter, Andreas Hofzumahaus, Anna Novelli, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 25, 3481–3502, https://doi.org/10.5194/acp-25-3481-2025, https://doi.org/10.5194/acp-25-3481-2025, 2025
Short summary
Short summary
Highly accurate rate coefficients of termolecular reactions between OH and HO2 radicals and reactive nitrogen oxides were measured for conditions in the lower troposphere, providing improved constraints on recommended values. No dependence on water vapour was found except for the HO2+NO2 reaction, which can be explained by an enhanced rate coefficient of the NO2 reaction with the water complex of the HO2 radical.
Hendrik Fuchs, Aaron Stainsby, Florian Berg, René Dubus, Michelle Färber, Andreas Hofzumahaus, Frank Holland, Kelvin H. Bates, Steven S. Brown, Matthew M. Coggon, Glenn S. Diskin, Georgios I. Gkatzelis, Christopher M. Jernigan, Jeff Peischl, Michael A. Robinson, Andrew W. Rollins, Nell B. Schafer, Rebecca H. Schwantes, Chelsea E. Stockwell, Patrick R. Veres, Carsten Warneke, Eleanor M. Waxman, Lu Xu, Kristen Zuraski, Andreas Wahner, and Anna Novelli
Atmos. Meas. Tech., 18, 881–895, https://doi.org/10.5194/amt-18-881-2025, https://doi.org/10.5194/amt-18-881-2025, 2025
Short summary
Short summary
Significant improvements have been made to the instruments used to measure OH reactivity, which is equivalent to the sum of air pollutant concentrations. Accurate and precise measurements with a high time resolution have been achieved, allowing use on aircraft, as demonstrated during flights in the USA.
Florian Berg, Anna Novelli, René Dubus, Andreas Hofzumahaus, Frank Holland, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 24, 13715–13731, https://doi.org/10.5194/acp-24-13715-2024, https://doi.org/10.5194/acp-24-13715-2024, 2024
Short summary
Short summary
This study reports temperature-dependent rate coefficients of the reaction of atmospherically relevant hydrocarbons from biogenic sources (methyl vinyl ketones and monoterpenes) and anthropogenic sources (alkanes and aromatics). Measurements were done at atmospheric conditions (ambient pressure and temperature range) in air.
Junwei Song, Georgios I. Gkatzelis, Ralf Tillmann, Nicolas Brüggemann, Thomas Leisner, and Harald Saathoff
Atmos. Chem. Phys., 24, 13199–13217, https://doi.org/10.5194/acp-24-13199-2024, https://doi.org/10.5194/acp-24-13199-2024, 2024
Short summary
Short summary
Biogenic volatile organic compounds (BVOCs) and organic aerosol (OA) particles were measured online in a stressed spruce-dominated forest. OA was mainly attributed to the monoterpene oxidation products. The mixing ratios of BVOCs were higher than the values previously measured in other temperate forests. The results demonstrate that BVOCs are influenced not only by meteorology and biogenic emissions but also by local anthropogenic emissions and subsequent chemical transformation processes.
Astrid Lampert, Rudolf Hankers, Thomas Feuerle, Thomas Rausch, Matthias Cremer, Maik Angermann, Mark Bitter, Jonas Füllgraf, Helmut Schulz, Ulf Bestmann, and Konrad B. Bärfuss
Earth Syst. Sci. Data, 16, 4777–4792, https://doi.org/10.5194/essd-16-4777-2024, https://doi.org/10.5194/essd-16-4777-2024, 2024
Short summary
Short summary
We conducted flights above the North Sea and investigated changes in the wind field. The research aircraft measured wind speed, wind direction, temperature, humidity and sea surface at high resolution. Wind parks reduce the wind speed, and the data help to determine how long it takes for the wind speed to recover. The coast also plays an important role, and the wind speed varies with distance from the coast. The results help in wind park planning and better estimating the energy yield.
Kuo-Ying Wang, Philippe Nedelec, Valerie Thouret, Hannah Clark, Andreas Wahner, and Andreas Petzold
EGUsphere, https://doi.org/10.5194/egusphere-2024-2414, https://doi.org/10.5194/egusphere-2024-2414, 2024
Preprint archived
Short summary
Short summary
We use routine in-service commercial passenger airplanes Airbus A340 and A330 to collect air pollutants in the upper troposphere. The beauty in using commercial airplanes is that these commercial airplanes, like taxi on the ground, keep flying all the time. We find that short-lived air pollutants are very sensitive to ground-level emissions. Effective regulation in ground-level emissions can help to reduce air pollution in the upper troposphere.
Hengheng Zhang, Christian Rolf, Ralf Tillmann, Christian Wesolek, Frank Gunther Wienhold, Thomas Leisner, and Harald Saathoff
Aerosol Research, 2, 135–151, https://doi.org/10.5194/ar-2-135-2024, https://doi.org/10.5194/ar-2-135-2024, 2024
Short summary
Short summary
Our study employs advanced tools, including scanning lidar, balloons, and UAVs, to explore aerosol particles in the atmosphere. The scanning lidar offers distinctive near-ground-level insights, enriching our comprehension of aerosol distribution from ground level to the free troposphere. This research provides valuable data for comparing remote sensing and in situ aerosol measurements, advancing our understanding of aerosol impacts on radiative transfer, clouds, and air quality.
Felix Wieser, Rolf Sander, Changmin Cho, Hendrik Fuchs, Thorsten Hohaus, Anna Novelli, Ralf Tillmann, and Domenico Taraborrelli
Geosci. Model Dev., 17, 4311–4330, https://doi.org/10.5194/gmd-17-4311-2024, https://doi.org/10.5194/gmd-17-4311-2024, 2024
Short summary
Short summary
The chemistry scheme of the atmospheric box model CAABA/MECCA is expanded to achieve an improved aerosol formation from emitted organic compounds. In addition to newly added reactions, temperature-dependent partitioning of all new species between the gas and aqueous phases is estimated and included in the pre-existing scheme. Sensitivity runs show an overestimation of key compounds from isoprene, which can be explained by a lack of aqueous-phase degradation reactions and box model limitations.
Yarê Baker, Sungah Kang, Hui Wang, Rongrong Wu, Jian Xu, Annika Zanders, Quanfu He, Thorsten Hohaus, Till Ziehm, Veronica Geretti, Thomas J. Bannan, Simon P. O'Meara, Aristeidis Voliotis, Mattias Hallquist, Gordon McFiggans, Sören R. Zorn, Andreas Wahner, and Thomas F. Mentel
Atmos. Chem. Phys., 24, 4789–4807, https://doi.org/10.5194/acp-24-4789-2024, https://doi.org/10.5194/acp-24-4789-2024, 2024
Short summary
Short summary
Highly oxygenated organic molecules are important contributors to secondary organic aerosol. Their yield depends on detailed atmospheric chemical composition. One important parameter is the ratio of hydroperoxy radicals to organic peroxy radicals (HO2/RO2), and we show that higher HO2/RO2 ratios lower the secondary organic aerosol yield. This is of importance as laboratory studies are often biased towards organic peroxy radicals.
Rongrong Wu, Sören R. Zorn, Sungah Kang, Astrid Kiendler-Scharr, Andreas Wahner, and Thomas F. Mentel
Atmos. Meas. Tech., 17, 1811–1835, https://doi.org/10.5194/amt-17-1811-2024, https://doi.org/10.5194/amt-17-1811-2024, 2024
Short summary
Short summary
Recent advances in high-resolution time-of-flight chemical ionization mass spectrometry (CIMS) enable the detection of highly oxygenated organic molecules, which efficiently contribute to secondary organic aerosol. Here we present an application of fuzzy c-means (FCM) clustering to deconvolve CIMS data. FCM not only reduces the complexity of mass spectrometric data but also the chemical and kinetic information retrieved by clustering gives insights into the chemical processes involved.
Barbara Harm-Altstädter, Konrad Bärfuss, Lutz Bretschneider, Martin Schön, Jens Bange, Ralf Käthner, Radovan Krejci, Mauro Mazzola, Kihong Park, Falk Pätzold, Alexander Peuker, Rita Traversi, Birgit Wehner, and Astrid Lampert
Aerosol Research, 1, 39–64, https://doi.org/10.5194/ar-1-39-2023, https://doi.org/10.5194/ar-1-39-2023, 2023
Short summary
Short summary
We present observations of aerosol particles and meteorological parameters in the horizontal and vertical distribution measured with uncrewed aerial systems in the Arctic. The field campaign was carried out during the snow melting season, when ultrafine aerosol particles (UFPs) with a size between 3 and 12 nm occurred frequently. A high variability of the measured UFPs was identified in the spatial scale, which was strongly associated with different atmospheric boundary layer properties.
Jacky Y. S. Pang, Florian Berg, Anna Novelli, Birger Bohn, Michelle Färber, Philip T. M. Carlsson, René Dubus, Georgios I. Gkatzelis, Franz Rohrer, Sergej Wedel, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 23, 12631–12649, https://doi.org/10.5194/acp-23-12631-2023, https://doi.org/10.5194/acp-23-12631-2023, 2023
Short summary
Short summary
In this study, the oxidations of sabinene by OH radicals and ozone were investigated with an atmospheric simulation chamber. Reaction rate coefficients of the OH-oxidation reaction at temperatures between 284 to 340 K were determined for the first time in the laboratory by measuring the OH reactivity. Product yields determined in chamber experiments had good agreement with literature values, but discrepancies were found between experimental yields and expected yields from oxidation mechanisms.
Konrad B. Bärfuss, Holger Schmithüsen, and Astrid Lampert
Atmos. Meas. Tech., 16, 3739–3765, https://doi.org/10.5194/amt-16-3739-2023, https://doi.org/10.5194/amt-16-3739-2023, 2023
Short summary
Short summary
The first atmospheric soundings with an electrically powered small uncrewed aircraft system (UAS) up to an altitude of 10 km are presented and assessed for quality, revealing the potential to augment atmospheric observations and fill observation gaps for numerical weather prediction. This is significant because of the need for high-resolution meteorological data, in particular in remote areas with limited in situ measurements, and for reference data for satellite measurement calibration.
Hao Luo, Luc Vereecken, Hongru Shen, Sungah Kang, Iida Pullinen, Mattias Hallquist, Hendrik Fuchs, Andreas Wahner, Astrid Kiendler-Scharr, Thomas F. Mentel, and Defeng Zhao
Atmos. Chem. Phys., 23, 7297–7319, https://doi.org/10.5194/acp-23-7297-2023, https://doi.org/10.5194/acp-23-7297-2023, 2023
Short summary
Short summary
Oxidation of limonene, an element emitted by trees and chemical products, by OH, a daytime oxidant, forms many highly oxygenated organic molecules (HOMs), including C10-20 compounds. HOMs play an important role in new particle formation and growth. HOM formation can be explained by the chemistry of peroxy radicals. We found that a minor branching ratio initial pathway plays an unexpected, significant role. Considering this pathway enables accurate simulations of HOMs and other concentrations.
Philip T. M. Carlsson, Luc Vereecken, Anna Novelli, François Bernard, Steven S. Brown, Bellamy Brownwood, Changmin Cho, John N. Crowley, Patrick Dewald, Peter M. Edwards, Nils Friedrich, Juliane L. Fry, Mattias Hallquist, Luisa Hantschke, Thorsten Hohaus, Sungah Kang, Jonathan Liebmann, Alfred W. Mayhew, Thomas Mentel, David Reimer, Franz Rohrer, Justin Shenolikar, Ralf Tillmann, Epameinondas Tsiligiannis, Rongrong Wu, Andreas Wahner, Astrid Kiendler-Scharr, and Hendrik Fuchs
Atmos. Chem. Phys., 23, 3147–3180, https://doi.org/10.5194/acp-23-3147-2023, https://doi.org/10.5194/acp-23-3147-2023, 2023
Short summary
Short summary
The investigation of the night-time oxidation of the most abundant hydrocarbon, isoprene, in chamber experiments shows the importance of reaction pathways leading to epoxy products, which could enhance particle formation, that have so far not been accounted for. The chemical lifetime of organic nitrates from isoprene is long enough for the majority to be further oxidized the next day by daytime oxidants.
Changmin Cho, Hendrik Fuchs, Andreas Hofzumahaus, Frank Holland, William J. Bloss, Birger Bohn, Hans-Peter Dorn, Marvin Glowania, Thorsten Hohaus, Lu Liu, Paul S. Monks, Doreen Niether, Franz Rohrer, Roberto Sommariva, Zhaofeng Tan, Ralf Tillmann, Astrid Kiendler-Scharr, Andreas Wahner, and Anna Novelli
Atmos. Chem. Phys., 23, 2003–2033, https://doi.org/10.5194/acp-23-2003-2023, https://doi.org/10.5194/acp-23-2003-2023, 2023
Short summary
Short summary
With this study, we investigated the processes leading to the formation, destruction, and recycling of radicals for four seasons in a rural environment. Complete knowledge of their chemistry is needed if we are to predict the formation of secondary pollutants from primary emissions. The results highlight a still incomplete understanding of the paths leading to the formation of the OH radical, which has been observed in several other environments as well and needs to be further investigated.
Tobias Schuldt, Georgios I. Gkatzelis, Christian Wesolek, Franz Rohrer, Benjamin Winter, Thomas A. J. Kuhlbusch, Astrid Kiendler-Scharr, and Ralf Tillmann
Atmos. Meas. Tech., 16, 373–386, https://doi.org/10.5194/amt-16-373-2023, https://doi.org/10.5194/amt-16-373-2023, 2023
Short summary
Short summary
We report in situ measurements of air pollutant concentrations within the planetary boundary layer on board a Zeppelin NT in Germany. We highlight the in-flight evaluation of electrochemical sensors that were installed inside a hatch box located on the bottom of the Zeppelin. Results from this work emphasize the potential of these sensors for other in situ airborne applications, e.g., on board unmanned aerial vehicles (UAVs).
Zhaofeng Tan, Hendrik Fuchs, Andreas Hofzumahaus, William J. Bloss, Birger Bohn, Changmin Cho, Thorsten Hohaus, Frank Holland, Chandrakiran Lakshmisha, Lu Liu, Paul S. Monks, Anna Novelli, Doreen Niether, Franz Rohrer, Ralf Tillmann, Thalassa S. E. Valkenburg, Vaishali Vardhan, Astrid Kiendler-Scharr, Andreas Wahner, and Roberto Sommariva
Atmos. Chem. Phys., 22, 13137–13152, https://doi.org/10.5194/acp-22-13137-2022, https://doi.org/10.5194/acp-22-13137-2022, 2022
Short summary
Short summary
During the 2019 JULIAC campaign, ClNO2 was measured at a rural site in Germany in different seasons. The highest ClNO2 level was 1.6 ppbv in September. ClNO2 production was more sensitive to the availability of NO2 than O3. The average ClNO2 production efficiency was up to 18 % in February and September and down to 3 % in December. These numbers are at the high end of the values reported in the literature, indicating the importance of ClNO2 chemistry in rural environments in midwestern Europe.
Yindong Guo, Hongru Shen, Iida Pullinen, Hao Luo, Sungah Kang, Luc Vereecken, Hendrik Fuchs, Mattias Hallquist, Ismail-Hakki Acir, Ralf Tillmann, Franz Rohrer, Jürgen Wildt, Astrid Kiendler-Scharr, Andreas Wahner, Defeng Zhao, and Thomas F. Mentel
Atmos. Chem. Phys., 22, 11323–11346, https://doi.org/10.5194/acp-22-11323-2022, https://doi.org/10.5194/acp-22-11323-2022, 2022
Short summary
Short summary
The oxidation of limonene, a common volatile emitted by trees and chemical products, by NO3, a nighttime oxidant, forms many highly oxygenated organic molecules (HOM), including C10-30 compounds. Most of the HOM are second-generation organic nitrates, in which carbonyl-substituted C10 nitrates accounted for a major fraction. Their formation can be explained by chemistry of peroxy radicals. HOM, especially low-volatile ones, play an important role in nighttime new particle formation and growth.
Jacky Yat Sing Pang, Anna Novelli, Martin Kaminski, Ismail-Hakki Acir, Birger Bohn, Philip T. M. Carlsson, Changmin Cho, Hans-Peter Dorn, Andreas Hofzumahaus, Xin Li, Anna Lutz, Sascha Nehr, David Reimer, Franz Rohrer, Ralf Tillmann, Robert Wegener, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 22, 8497–8527, https://doi.org/10.5194/acp-22-8497-2022, https://doi.org/10.5194/acp-22-8497-2022, 2022
Short summary
Short summary
This study investigates the radical chemical budget during the limonene oxidation at different atmospheric-relevant NO concentrations in chamber experiments under atmospheric conditions. It is found that the model–measurement discrepancies of HO2 and RO2 are very large at low NO concentrations that are typical for forested environments. Possible additional processes impacting HO2 and RO2 concentrations are discussed.
Ralf Tillmann, Georgios I. Gkatzelis, Franz Rohrer, Benjamin Winter, Christian Wesolek, Tobias Schuldt, Anne C. Lange, Philipp Franke, Elmar Friese, Michael Decker, Robert Wegener, Morten Hundt, Oleg Aseev, and Astrid Kiendler-Scharr
Atmos. Meas. Tech., 15, 3827–3842, https://doi.org/10.5194/amt-15-3827-2022, https://doi.org/10.5194/amt-15-3827-2022, 2022
Short summary
Short summary
We report in situ measurements of air pollutant concentrations within the planetary boundary layer on board a Zeppelin in Germany. The low costs of commercial flights provide an affordable and efficient method to improve our understanding of changes in emissions in space and time. The experimental setup expands the capabilities of this platform and provides insights into primary and secondary pollution observations and planetary boundary layer dynamics which determine air quality significantly.
Beatriz Cañadillas, Maximilian Beckenbauer, Juan J. Trujillo, Martin Dörenkämper, Richard Foreman, Thomas Neumann, and Astrid Lampert
Wind Energ. Sci., 7, 1241–1262, https://doi.org/10.5194/wes-7-1241-2022, https://doi.org/10.5194/wes-7-1241-2022, 2022
Short summary
Short summary
Scanning lidar measurements combined with meteorological sensors and mesoscale simulations reveal the strong directional and stability dependence of the wake strength in the direct vicinity of wind farm clusters.
Philipp Franke, Anne Caroline Lange, and Hendrik Elbern
Geosci. Model Dev., 15, 1037–1060, https://doi.org/10.5194/gmd-15-1037-2022, https://doi.org/10.5194/gmd-15-1037-2022, 2022
Short summary
Short summary
The paper proposes an ensemble-based analysis framework (ESIAS-chem) for time- and altitude-resolved volcanic ash emission fluxes and their uncertainty. The core of the algorithm is an ensemble Nelder–Mead optimization algorithm accompanied by a particle filter update. The performed notional experiments demonstrate the high accuracy of ESIAS-chem in analyzing the vertically resolved volcanic ash in the atmosphere. Further, the system is in general able to estimate the emission fluxes properly.
Zhaofeng Tan, Luisa Hantschke, Martin Kaminski, Ismail-Hakki Acir, Birger Bohn, Changmin Cho, Hans-Peter Dorn, Xin Li, Anna Novelli, Sascha Nehr, Franz Rohrer, Ralf Tillmann, Robert Wegener, Andreas Hofzumahaus, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 21, 16067–16091, https://doi.org/10.5194/acp-21-16067-2021, https://doi.org/10.5194/acp-21-16067-2021, 2021
Short summary
Short summary
The photo-oxidation of myrcene, a monoterpene species emitted by plants, was investigated at atmospheric conditions in the outdoor simulation chamber SAPHIR. The chemical structure of myrcene is partly similar to isoprene. Therefore, it can be expected that hydrogen shift reactions could play a role as observed for isoprene. In this work, their potential impact on the regeneration efficiency of hydroxyl radicals is investigated.
Janne Lampilahti, Hanna E. Manninen, Tuomo Nieminen, Sander Mirme, Mikael Ehn, Iida Pullinen, Katri Leino, Siegfried Schobesberger, Juha Kangasluoma, Jenni Kontkanen, Emma Järvinen, Riikka Väänänen, Taina Yli-Juuti, Radovan Krejci, Katrianne Lehtipalo, Janne Levula, Aadu Mirme, Stefano Decesari, Ralf Tillmann, Douglas R. Worsnop, Franz Rohrer, Astrid Kiendler-Scharr, Tuukka Petäjä, Veli-Matti Kerminen, Thomas F. Mentel, and Markku Kulmala
Atmos. Chem. Phys., 21, 12649–12663, https://doi.org/10.5194/acp-21-12649-2021, https://doi.org/10.5194/acp-21-12649-2021, 2021
Short summary
Short summary
We studied aerosol particle formation and growth in different parts of the planetary boundary layer at two different locations (Po Valley, Italy, and Hyytiälä, Finland). The observations consist of airborne measurements on board an instrumented Zeppelin and a small airplane combined with comprehensive ground-based measurements.
Luisa Hantschke, Anna Novelli, Birger Bohn, Changmin Cho, David Reimer, Franz Rohrer, Ralf Tillmann, Marvin Glowania, Andreas Hofzumahaus, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 21, 12665–12685, https://doi.org/10.5194/acp-21-12665-2021, https://doi.org/10.5194/acp-21-12665-2021, 2021
Short summary
Short summary
The reactions of Δ3-carene with ozone and the hydroxyl radical (OH) and the photolysis and OH reaction of caronaldehyde were investigated in the simulation chamber SAPHIR. Reaction rate constants of these reactions were determined. Caronaldehyde yields of the ozonolysis and OH reaction were determined. The organic nitrate yield of the reaction of Δ3-carene and caronaldehyde-derived peroxy radicals with NO was determined. The ROx budget (ROx = OH+HO2+RO2) was also investigated.
Simon Rosanka, Bruno Franco, Lieven Clarisse, Pierre-François Coheur, Andrea Pozzer, Andreas Wahner, and Domenico Taraborrelli
Atmos. Chem. Phys., 21, 11257–11288, https://doi.org/10.5194/acp-21-11257-2021, https://doi.org/10.5194/acp-21-11257-2021, 2021
Short summary
Short summary
The strong El Niño in 2015 led to a particular dry season in Indonesia and favoured severe peatland fires. The smouldering conditions of these fires and the high carbon content of peat resulted in high volatile organic compound (VOC) emissions. By using a comprehensive atmospheric model, we show that these emissions have a significant impact on the tropospheric composition and oxidation capacity. These emissions are transported into to the lower stratosphere, resulting in a depletion of ozone.
Rongrong Wu, Luc Vereecken, Epameinondas Tsiligiannis, Sungah Kang, Sascha R. Albrecht, Luisa Hantschke, Defeng Zhao, Anna Novelli, Hendrik Fuchs, Ralf Tillmann, Thorsten Hohaus, Philip T. M. Carlsson, Justin Shenolikar, François Bernard, John N. Crowley, Juliane L. Fry, Bellamy Brownwood, Joel A. Thornton, Steven S. Brown, Astrid Kiendler-Scharr, Andreas Wahner, Mattias Hallquist, and Thomas F. Mentel
Atmos. Chem. Phys., 21, 10799–10824, https://doi.org/10.5194/acp-21-10799-2021, https://doi.org/10.5194/acp-21-10799-2021, 2021
Short summary
Short summary
Isoprene is the biogenic volatile organic compound with the largest emissions rates. The nighttime reaction of isoprene with the NO3 radical has a large potential to contribute to SOA. We classified isoprene nitrates into generations and proposed formation pathways. Considering the potential functionalization of the isoprene nitrates we propose that mainly isoprene dimers contribute to SOA formation from the isoprene NO3 reactions with at least a 5 % mass yield.
Simon Rosanka, Rolf Sander, Andreas Wahner, and Domenico Taraborrelli
Geosci. Model Dev., 14, 4103–4115, https://doi.org/10.5194/gmd-14-4103-2021, https://doi.org/10.5194/gmd-14-4103-2021, 2021
Short summary
Short summary
The Jülich Aqueous-phase Mechanism of Organic Chemistry (JAMOC) is developed and implemented into the Module Efficiently Calculating the Chemistry of the Atmosphere (MECCA). JAMOC is an explicit in-cloud oxidation scheme for oxygenated volatile organic compounds (OVOCs), which is suitable for global model applications. Within a box-model study, we show that JAMOC yields reduced gas-phase concentrations of most OVOCs and oxidants, except for nitrogen oxides.
Simon Rosanka, Rolf Sander, Bruno Franco, Catherine Wespes, Andreas Wahner, and Domenico Taraborrelli
Atmos. Chem. Phys., 21, 9909–9930, https://doi.org/10.5194/acp-21-9909-2021, https://doi.org/10.5194/acp-21-9909-2021, 2021
Short summary
Short summary
In-cloud destruction of ozone depends on hydroperoxyl radicals in cloud droplets, where they are produced by oxygenated volatile organic compound (OVOC) oxygenation. Only rudimentary representations of these processes, if any, are currently available in global atmospheric models. By using a comprehensive atmospheric model that includes a complex in-cloud OVOC oxidation scheme, we show that atmospheric oxidants are reduced and models ignoring this process will underpredict clouds as ozone sinks.
Defeng Zhao, Iida Pullinen, Hendrik Fuchs, Stephanie Schrade, Rongrong Wu, Ismail-Hakki Acir, Ralf Tillmann, Franz Rohrer, Jürgen Wildt, Yindong Guo, Astrid Kiendler-Scharr, Andreas Wahner, Sungah Kang, Luc Vereecken, and Thomas F. Mentel
Atmos. Chem. Phys., 21, 9681–9704, https://doi.org/10.5194/acp-21-9681-2021, https://doi.org/10.5194/acp-21-9681-2021, 2021
Short summary
Short summary
The reaction of isoprene, a biogenic volatile organic compound with the globally largest emission rates, with NO3, an nighttime oxidant influenced heavily by anthropogenic emissions, forms a large number of highly oxygenated organic molecules (HOM). These HOM are formed via one or multiple oxidation steps, followed by autoxidation. Their total yield is much higher than that in the daytime oxidation of isoprene. They may play an important role in nighttime organic aerosol formation and growth.
Marvin Glowania, Franz Rohrer, Hans-Peter Dorn, Andreas Hofzumahaus, Frank Holland, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Meas. Tech., 14, 4239–4253, https://doi.org/10.5194/amt-14-4239-2021, https://doi.org/10.5194/amt-14-4239-2021, 2021
Short summary
Short summary
Three instruments that use different techniques to measure gaseous formaldehyde concentrations were compared in experiments in the atmospheric simulation chamber SAPHIR at Forschungszentrum Jülich. The results demonstrated the need to correct the baseline in measurements by instruments that use the Hantzsch reaction or make use of cavity ring-down spectroscopy. After applying corrections, all three methods gave accurate and precise measurements within their specifications.
Michael Priestley, Thomas J. Bannan, Michael Le Breton, Stephen D. Worrall, Sungah Kang, Iida Pullinen, Sebastian Schmitt, Ralf Tillmann, Einhard Kleist, Defeng Zhao, Jürgen Wildt, Olga Garmash, Archit Mehra, Asan Bacak, Dudley E. Shallcross, Astrid Kiendler-Scharr, Åsa M. Hallquist, Mikael Ehn, Hugh Coe, Carl J. Percival, Mattias Hallquist, Thomas F. Mentel, and Gordon McFiggans
Atmos. Chem. Phys., 21, 3473–3490, https://doi.org/10.5194/acp-21-3473-2021, https://doi.org/10.5194/acp-21-3473-2021, 2021
Short summary
Short summary
A significant fraction of emissions from human activity consists of aromatic hydrocarbons, e.g. benzene, which oxidise to form new compounds important for particle growth. Characterisation of benzene oxidation products highlights the range of species produced as well as their chemical properties and contextualises them within relevant frameworks, e.g. MCM. Cluster analysis of the oxidation product time series distinguishes behaviours of CHON compounds that could aid in identifying functionality.
Changmin Cho, Andreas Hofzumahaus, Hendrik Fuchs, Hans-Peter Dorn, Marvin Glowania, Frank Holland, Franz Rohrer, Vaishali Vardhan, Astrid Kiendler-Scharr, Andreas Wahner, and Anna Novelli
Atmos. Meas. Tech., 14, 1851–1877, https://doi.org/10.5194/amt-14-1851-2021, https://doi.org/10.5194/amt-14-1851-2021, 2021
Short summary
Short summary
This study describes the implementation and characterization of the chemical modulation reactor (CMR) used in the laser-induced fluorescence instrument of the Forschungszentrum Jülich. The CMR allows for interference-free OH radical measurement in ambient air. During a field campaign in a rural environment, the observed interference was mostly below the detection limit of the instrument and fully explained by the known ozone interference.
Cited articles
Ackermann, I. J., Hass, H., Memmesheimer, M., Ebel, A., Binkowski, F. S., and Shankar, U.: Modal aerosol dynamics model for Europe: development and first applications, Atmos. Environ., 32, 2981–2999, https://doi.org/10.1016/S1352-2310(98)00006-5, 1998. a
Altstädter, B., Platis, A., Wehner, B., Scholtz, A., Wildmann, N., Hermann, M., Käthner, R., Baars, H., Bange, J., and Lampert, A.: ALADINA - an unmanned research aircraft for observing vertical and horizontal distributions of ultrafine particles within the atmospheric boundary layer, Atmos. Meas. Tech., 8, 1627–1639, https://doi.org/10.5194/amt-8-1627-2015, 2015. a
Bretschneider, L., Schlerf, A., Baum, A., Bohlius, H., Buchholz, M., Düsing, S., Ebert, V., Erraji, H., Frost, P., Käthner, R., Krüger, T., Lange, A. C., Langner, M., Nowak, A., Pätzold, F., Rüdiger, J., Saturno, J., Scholz, H., Schuldt, T., Seldschopf, R., Sobotta, A., Tillmann, R., Wehner, B., Wesolek, C., Wolf, K., and Lampert, A.: MesSBAR-Multicopter and Instrumentation for Air Quality Research, Atmosphere, 13, 629, https://doi.org/10.3390/atmos13040629, 2022. a, b
Corrigan, C. E., Roberts, G. C., Ramana, M. V., Kim, D., and Ramanathan, V.: Capturing vertical profiles of aerosols and black carbon over the Indian Ocean using autonomous unmanned aerial vehicles, Atmos. Chem. Phys., 8, 737–747, https://doi.org/10.5194/acp-8-737-2008, 2008. a
De Mazière, M., Thompson, A. M., Kurylo, M. J., Wild, J. D., Bernhard, G., Blumenstock, T., Braathen, G. O., Hannigan, J. W., Lambert, J.-C., Leblanc, T., McGee, T. J., Nedoluha, G., Petropavlovskikh, I., Seckmeyer, G., Simon, P. C., Steinbrecht, W., and Strahan, S. E.: The Network for the Detection of Atmospheric Composition Change (NDACC): history, status and perspectives, Atmos. Chem. Phys., 18, 4935–4964, https://doi.org/10.5194/acp-18-4935-2018, 2018. a
Deroubaix, A., Hoelzemann, J. J., Ynoue, R. Y., de Almeida Albuquerque, T. T., Alves, R. C., de Fatima Andrade, M., ao, W. L. A., Bouarar, I., de Souza Fernandes Duarte, E., Elbern, H., Franke, P., Lange, A. C., Lichtig, P., Lugon, L., Martins, L. D., de Arruda Moreira, G., Pedruzzi, R., Rosario, N., and Brasseur, G.: Intercomparison of Air Quality Models in a Megacity: Toward an Operational Ensemble Forecasting System for São Paulo, J. Geophys. Res.-Atmos., 129, e2022JD038179, https://doi.org/10.1029/2022JD038179, 2024. a
Diaz, J., Corrales, E., Madrigal, Y., Pieri, D., Bland, G., Miles, T., and Fladeland, M.: Volcano Monitoring with small Unmanned Aerial Systems, American Institute of Aeronautics and Astronautics, ISBN 978-1-60086-939-6, https://doi.org/10.2514/6.2012-2522, 2012. a
Duarte, E. D. S. F., Franke, P., Lange, A. C., Friese, E., da Silva Lopes, F. J., ao da Silva, J. J., dos Reis, J. S., Landulfo, E., e Silva, C. M. S., Elbern, H., and Hoelzemann, J. J.: Evaluation of atmospheric aerosols in the metropolitan area of São Paulo simulated by the regional EURAD-IM model on high-resolution, Atmos. Pollut. Res., 12, 451–469, https://doi.org/10.1016/j.apr.2020.12.006, 2021. a
Elbern, H. and Schmidt, H.: Ozone episode analysis by four-dimensional variational chemistry data assimilation, J. Geophys. Res.-Atmos., 106, 3569–3590, https://doi.org/10.1029/2000JD900448, 2001. a
Flagg, D. D., Doyle, J. D., Holt, T. R., Tyndall, D. P., Amerault, C. M., Geiszler, D., Haack, T., Moskaitis, J. R., Nachamkin, J., and Eleuterio, D. P.: On the Impact of Unmanned Aerial System Observations on Numerical Weather Prediction in the Coastal Zone, Mon. Weather Rev., 146, 599–622, https://doi.org/10.1175/MWR-D-17-0028.1, 2018. a, b
Franke, P., Lange, A. C., and Elbern, H.: Particle-filter-based volcanic ash emission inversion applied to a hypothetical sub-Plinian Eyjafjallajökull eruption using the Ensemble for Stochastic Integration of Atmospheric Simulations (ESIAS-chem) version 1.0, Geosci. Model Dev., 15, 1037–1060, https://doi.org/10.5194/gmd-15-1037-2022, 2022. a
Franke, P., Lange, A. C., Steffens, B., Pozzer, A., Wahner, A., and Kiendler-Scharr, A.: European air quality in view of the WHO 2021 guideline levels: Effect of emission reductions on air pollution exposure, Elem. Sci. Anth., 12, 00127, https://doi.org/10.1525/elementa.2023.00127, 2024. a
Gama, C., Ribeiro, I., Lange, A. C., Vogel, A., Ascenso, A., Seixas, V., Elbern, H., Borrego, C., Friese, E., and Monteiro, A.: Performance assessment of CHIMERE and EURAD-IM' dust modules, Atmos. Pollut. Res., 10, 1336–1346, https://doi.org/10.1016/j.apr.2019.03.005, 2019. a
García, O. E., Schneider, M., Sepúlveda, E., Hase, F., Blumenstock, T., Cuevas, E., Ramos, R., Gross, J., Barthlott, S., Röhling, A. N., Sanromá, E., González, Y., Gómez-Peláez, Á. J., Navarro-Comas, M., Puentedura, O., Yela, M., Redondas, A., Carreño, V., León-Luis, S. F., Reyes, E., García, R. D., Rivas, P. P., Romero-Campos, P. M., Torres, C., Prats, N., Hernández, M., and López, C.: Twenty years of ground-based NDACC FTIR spectrometry at Izaña Observatory – overview and long-term comparison to other techniques, Atmos. Chem. Phys., 21, 15519–15554, https://doi.org/10.5194/acp-21-15519-2021, 2021. a
Guenther, A. B., Jiang, X., Heald, C. L., Sakulyanontvittaya, T., Duhl, T., Emmons, L. K., and Wang, X.: The Model of Emissions of Gases and Aerosols from Nature version 2.1 (MEGAN2.1): an extended and updated framework for modeling biogenic emissions, Geosci. Model Dev., 5, 1471–1492, https://doi.org/10.5194/gmd-5-1471-2012, 2012. a
Illingworth, S., Allen, G., Percival, C., Hollingsworth, P., Gallagher, M., Ricketts, H., Hayes, H., Ładosz, P., Crawley, D., and Roberts, G.: Measurement of boundary layer ozone concentrations on-board a Skywalker unmanned aerial vehicle, Atmos. Sci. Lett., 15, 252–258, https://doi.org/10.1002/asl2.496, 2014. a
Jensen, A. A., Pinto, J. O., Bailey, S. C. C., Sobash, R. A., de Boer, G., Houston, A. L., Chilson, P. B., Bell, T., Romine, G., Smith, S. W., Lawrence, D. A., Dixon, C., Lundquist, J. K., Jacob, J. D., Elston, J., Waugh, S., and Steiner, M.: Assimilation of a Coordinated Fleet of Uncrewed Aircraft System Observations in Complex Terrain: EnKF System Design and Preliminary Assessment, Mon. Weather Rev., 149, 1459–1480, https://doi.org/10.1175/MWR-D-20-0359.1, 2021. a
Jonassen, M. O., Ólafsson, H., Ágústsson, H., Ólafur Rögnvaldsson, and Reuder, J.: Improving High-Resolution Numerical Weather Simulations by Assimilating Data from an Unmanned Aerial System, Mon. Weather Rev., 140, 3734–3756, https://doi.org/10.1175/MWR-D-11-00344.1, 2012. a
Jülich Supercomputing Centre: JURECA: Data Centric and Booster Modules implementing the Modular Supercomputing Architecture at Jülich Supercomputing Centre, J. Large-Scale Res. Facil. JLSRF, 7, A182, https://doi.org/10.17815/jlsrf-7-182, 2021. a
Klonecki, A., Pommier, M., Clerbaux, C., Ancellet, G., Cammas, J.-P., Coheur, P.-F., Cozic, A., Diskin, G. S., Hadji-Lazaro, J., Hauglustaine, D. A., Hurtmans, D., Khattatov, B., Lamarque, J.-F., Law, K. S., Nedelec, P., Paris, J.-D., Podolske, J. R., Prunet, P., Schlager, H., Szopa, S., and Turquety, S.: Assimilation of IASI satellite CO fields into a global chemistry transport model for validation against aircraft measurements, Atmos. Chem. Phys., 12, 4493–4512, https://doi.org/10.5194/acp-12-4493-2012, 2012. a
Kuenen, J. J. P., Visschedijk, A. J. H., Jozwicka, M., and Denier van der Gon, H. A. C.: TNO-MACC_II emission inventory; a multi-year (2003–2009) consistent high-resolution European emission inventory for air quality modelling, Atmos. Chem. Phys., 14, 10963–10976, https://doi.org/10.5194/acp-14-10963-2014, 2014. a, b
Lampert, A., Altstädter, B., Bärfuss, K., Bretschneider, L., Sandgaard, J., Michaelis, J., Lobitz, L., Asmussen, M., Damm, E., Käthner, R., Krüger, T., Lüpkes, C., Nowak, S., Peuker, A., Rausch, T., Reiser, F., Scholtz, A., Zakharov, D. S., Gaus, D., Bansmer, S., Wehner, B., and Pätzold, F.: Unmanned Aerial Systems for Investigating the Polar Atmospheric Boundary Layer – Technical Challenges and Examples of Applications, Atmosphere, 11, 416, https://doi.org/10.3390/atmos11040416, 2020. a
Lawrence, D. A. and Balsley, B. B.: High-Resolution Atmospheric Sensing of Multiple Atmospheric Variables Using the DataHawk Small Airborne Measurement System, J. Atmos. Ocean. Technol., 30, 2352–2366, https://doi.org/10.1175/JTECH-D-12-00089.1, 2013. a
Leuenberger, D., Haefele, A., Omanovic, N., Fengler, M., Martucci, G., Calpini, B., Fuhrer, O., and Rossa, A.: Improving High-Impact Numerical Weather Prediction with Lidar and Drone Observations, B. Am. Meteorol. Soc., 101, E1036–E1051, https://doi.org/10.1175/BAMS-D-19-0119.1, 2020. a, b
Liu, D. C. and Nocedal, J.: On the limited memory BFGS method for large scale optimization, Math. Program., 45, 503–528, https://doi.org/10.1007/BF01589116, 1989. a, b
Liu, X., Mizzi, A. P., Anderson, J. L., Fung, I. Y., and Cohen, R. C.: Assimilation of satellite NO2 observations at high spatial resolution using OSSEs, Atmos. Chem. Phys., 17, 7067–7081, https://doi.org/10.5194/acp-17-7067-2017, 2017. a
Marécal, V., Peuch, V.-H., Andersson, C., Andersson, S., Arteta, J., Beekmann, M., Benedictow, A., Bergström, R., Bessagnet, B., Cansado, A., Chéroux, F., Colette, A., Coman, A., Curier, R. L., Denier van der Gon, H. A. C., Drouin, A., Elbern, H., Emili, E., Engelen, R. J., Eskes, H. J., Foret, G., Friese, E., Gauss, M., Giannaros, C., Guth, J., Joly, M., Jaumouillé, E., Josse, B., Kadygrov, N., Kaiser, J. W., Krajsek, K., Kuenen, J., Kumar, U., Liora, N., Lopez, E., Malherbe, L., Martinez, I., Melas, D., Meleux, F., Menut, L., Moinat, P., Morales, T., Parmentier, J., Piacentini, A., Plu, M., Poupkou, A., Queguiner, S., Robertson, L., Rouïl, L., Schaap, M., Segers, A., Sofiev, M., Tarasson, L., Thomas, M., Timmermans, R., Valdebenito, A., van Velthoven, P., van Versendaal, R., Vira, J., and Ung, A.: A regional air quality forecasting system over Europe: the MACC-II daily ensemble production, Geosci. Model Dev., 8, 2777–2813, https://doi.org/10.5194/gmd-8-2777-2015, 2015. a
Martin, R. V.: Satellite remote sensing of surface air quality, Atmos. Environ., 42, 7823–7843, https://doi.org/10.1016/j.atmosenv.2008.07.018, 2008. a
Memmesheimer, M., H. Hass, J. Tippke, and A. Ebel: Modeling of episodic emission data for Europe with the EURAD Emission Model EEM, in: the International Speciality Conference “Regional Photochemical Measurement and modeling studies”, San Diego, CA, USA, 101 pp., Vol. 2, edited by: Ranzieri, A. and Solomon, P., 495–499 pp., Air and Waste Management Association, 1995. a
Menut, L., Goussebaile, A., Bessagnet, B., Khvorostiyanov, D., and Ung, A.: Impact of realistic hourly emissions profiles on air pollutants concentrations modelled with CHIMERE, Atmos. Environ., 49, 233–244, https://doi.org/10.1016/j.atmosenv.2011.11.057, 2012. a
Nathan, B. J., Golston, L. M., O'Brien, A. S., Ross, K., Harrison, W. A., Tao, L., Lary, D. J., Johnson, D. R., Covington, A. N., Clark, N. N., and Zondlo, M. A.: Near-Field Characterization of Methane Emission Variability from a Compressor Station Using a Model Aircraft, Environ. Sci. Technol., 49, 7896–7903, https://doi.org/10.1021/acs.est.5b00705, 2015. a
O'Sullivan, D., Taylor, S., Elston, J., Baker, C. B., Hotz, D., Marshall, C., Jacob, J., Barfuss, K., Piguet, B., Roberts, G., Omanovic, N., Fengler, M., Jensen, A. A., Steiner, M., and Houston, A. L.: The Status and Future of Small Uncrewed Aircraft Systems (UAS) in Operational Meteorology, B. Am. Meteorol. Soc., 102, E2121–E2136, https://doi.org/10.1175/BAMS-D-20-0138.1, 2021. a
Paschalidi, Z.: Inverse Modelling for Tropospheric Chemical State Estimation by 4-Dimensional Variational Data Assimilation from Routinely and Campaign Platforms, Ph.D. thesis, University of Cologne, 101 pp., https://kups.ub.uni-koeln.de/6588/ (last access: 27 November 2024), 2015. a
Petetin, H., Jeoffrion, M., Sauvage, B., Athier, G., Blot, R., Boulanger, D., Clark, H., Cousin, J.-M., Gheusi, F., Nedelec, P., Steinbacher, M., and Thouret, V.: Representativeness of the IAGOS airborne measurements in the lower troposphere, Elementa-Sci. Anthrop., 6, 23, https://doi.org/10.1525/elementa.280, 2018. a
Rabitz, H. and Aliş, O. F.: General foundations of high-dimensional model representations, J. Math. Chem., 25, 197–233, https://doi.org/10.1023/A:1019188517934, 1999. a
Roberts, G. C., Ramana, M. V., Corrigan, C., Kim, D., and Ramanathan, V.: Simultaneous observations of aerosol-cloud-albedo interactions with three stacked unmanned aerial vehicles, P. Natl. Acad. Sci. USA, 105, 7370–7375, https://doi.org/10.1073/pnas.0710308105, 2008. a
Roselle, S. and Binkowski, F.: Cloud Dynamics and Chemistry, in Science Algorithms of the EPA Models-3 Community Multiscale Air Quality (CMAQ) Modeling System, Research Triangle Park, EPA 600/R-99-030, https://www.cmascenter.org/cmaq/science_documentation/pdf/ch11.pdf (last access: 27 November 2024), 1999. a
Sandu, A. and Sander, R.: Technical note: Simulating chemical systems in Fortran90 and Matlab with the Kinetic PreProcessor KPP-2.1, Atmos. Chem. Phys, 6, 187–195, https://doi.org/10.5194/acp-6-187-2006, 2006. a
Scheffe, R., Philbrick, R., on Macdonald, C., Dye, T., Gilroy, M., and Carlton, A.-M.: Observational Needs for Four-dimensional Air Quality Characterization, https://cfpub.epa.gov/si/si_public_record_report.cfm?Lab=NERL&dirEntryId=213564 (last access: 27 November 2024), 2009. a
Schell, B., Ackermann, I. J., Hass, H., Binkowski, F. S., and Ebel, A.: Modeling the formation of secondary organic aerosol within a comprehensive air quality model system, J. Geophys. Res.-Atmos., 106, 28275–28293, https://doi.org/10.1029/2001JD000384, 2001. a
Schlerf, A., Bretschneider, L., Schuchard, M., Düsing, S., Käthner, R., Wehner, B., Schuldt, T., Wesolek, C., Tillmann, R., Lange, A. C., Erraji, H., Krüger, T., Scholz, H., Frost, P., Sobotta, A., Baum, A., Ebert, V., Bohlius, H., Nowak, A., Langner, M., and Lampert, A.: Validation and optimization of the drone air quality measurement system MesSBAR, Pangaea [data set], https://doi.org/10.1594/PANGAEA.971503, 2024. a, b
Schuldt, T., Gkatzelis, G. I., Wesolek, C., Rohrer, F., Winter, B., Kuhlbusch, T. A. J., Kiendler-Scharr, A., and Tillmann, R.: Electrochemical sensors on board a Zeppelin NT: in-flight evaluation of low-cost trace gas measurements, Atmos. Meas. Tech., 16, 373–386, https://doi.org/10.5194/amt-16-373-2023, 2023. a
Schuyler, T. and Guzman, M.: Unmanned Aerial Systems for Monitoring Trace Tropospheric Gases, Atmosphere, 8, 206, https://doi.org/10.3390/atmos8100206, 2017. a
Sillman, S.: The relation between ozone, NOx and hydrocarbons in urban and polluted rural environments, Atmos. Environ., 33, 1821–1845, https://doi.org/10.1016/S1352-2310(98)00345-8, 1999. a, b
Skamarock, W. C., Klemp, J. B., Dudhia, J., Gill, D. O., Barker, D. M., Duda, M. G., Huang, X.-Y., Wang, W., and Powers, J. G.: A Description of the Advanced Research WRF Version 3, https://doi.org/10.5065/D68S4MVH, 2008. a
Stockwell, W. R., Kirchner, F., Kuhn, M., and Seefeld, S.: A new mechanism for regional atmospheric chemistry modeling, J. Geophys. Res., 102, 847–872, https://doi.org/10.1029/97JD00849, 1997. a
Sun, Q., Vihma, T., Jonassen, M. O., and Zhang, Z.: Impact of Assimilation of Radiosonde and UAV Observations from the Southern Ocean in the Polar WRF Model, Adv. Atmos. Sci., 37, 441–454, https://doi.org/10.1007/s00376-020-9213-8, 2020. a
Tillmann, R., Gkatzelis, G. I., Rohrer, F., Winter, B., Wesolek, C., Schuldt, T., Lange, A. C., Franke, P., Friese, E., Decker, M., Wegener, R., Hundt, M., Aseev, O., and Kiendler-Scharr, A.: Air quality observations onboard commercial and targeted Zeppelin flights in Germany – a platform for high-resolution trace-gas and aerosol measurements within the planetary boundary layer, Atmos. Meas. Tech., 15, 3827–3842, https://doi.org/10.5194/amt-15-3827-2022, 2022. a, b
Tirpitz, J.-L., Frieß, U., Hendrick, F., Alberti, C., Allaart, M., Apituley, A., Bais, A., Beirle, S., Berkhout, S., Bognar, K., Bösch, T., Bruchkouski, I., Cede, A., Chan, K. L., den Hoed, M., Donner, S., Drosoglou, T., Fayt, C., Friedrich, M. M., Frumau, A., Gast, L., Gielen, C., Gomez-Martín, L., Hao, N., Hensen, A., Henzing, B., Hermans, C., Jin, J., Kreher, K., Kuhn, J., Lampel, J., Li, A., Liu, C., Liu, H., Ma, J., Merlaud, A., Peters, E., Pinardi, G., Piters, A., Platt, U., Puentedura, O., Richter, A., Schmitt, S., Spinei, E., Stein Zweers, D., Strong, K., Swart, D., Tack, F., Tiefengraber, M., van der Hoff, R., van Roozendael, M., Vlemmix, T., Vonk, J., Wagner, T., Wang, Y., Wang, Z., Wenig, M., Wiegner, M., Wittrock, F., Xie, P., Xing, C., Xu, J., Yela, M., Zhang, C., and Zhao, X.: Intercomparison of MAX-DOAS vertical profile retrieval algorithms: studies on field data from the CINDI-2 campaign, Atmos. Meas. Tech., 14, 1–35, https://doi.org/10.5194/amt-14-1-2021, 2021. a
Villa, T., Gonzalez, F., Miljievic, B., Ristovski, Z., and Morawska, L.: An Overview of Small Unmanned Aerial Vehicles for Air Quality Measurements: Present Applications and Future Prospectives, Sensors, 16, 1072, https://doi.org/10.3390/s16071072, 2016. a
Visser, A. J., Boersma, K. F., Ganzeveld, L. N., and Krol, M. C.: European NOx emissions in WRF-Chem derived from OMI: impacts on summertime surface ozone, Atmos. Chem. Phys., 19, 11821–11841, https://doi.org/10.5194/acp-19-11821-2019, 2019. a
Walcek, C. J.: Minor flux adjustment near mixing ratio extremes for simplified yet highly accurate monotonic calculation of tracer advection, J. Geophys. Res.-Atmos., 105, 9335–9348, https://doi.org/10.1029/1999JD901142, 2000. a
Wang, H., Lu, X., Jacob, D. J., Cooper, O. R., Chang, K.-L., Li, K., Gao, M., Liu, Y., Sheng, B., Wu, K., Wu, T., Zhang, J., Sauvage, B., Nédélec, P., Blot, R., and Fan, S.: Global tropospheric ozone trends, attributions, and radiative impacts in 1995–2017: an integrated analysis using aircraft (IAGOS) observations, ozonesonde, and multi-decadal chemical model simulations, Atmos. Chem. Phys., 22, 13753–13782, https://doi.org/10.5194/acp-22-13753-2022, 2022. a
Wang, Y.-C., Wang, S.-H., Lewis, J. R., Chang, S.-C., and Griffith, S. M.: Determining Planetary Boundary Layer Height by Micro-pulse Lidar with Validation by UAV Measurements, Aerosol. Air. Qual. Res., 21, 200336, https://doi.org/10.4209/aaqr.200336, 2021. a
Weaver, A. and Courtier, P.: Correlation modelling on the sphere using a generalized diffusion equation, Q. J. Roy. Meteor. Soc., 127, 1815–1846, https://doi.org/10.1002/qj.49712757518, 2001. a, b
Wu, X., Elbern, H., and Jacob, B.: The assessment of potential observability for joint chemical states and emissions in atmospheric modelings, Stoch. Environ. Res. Risk. Assess., 36, 1743–1760, https://doi.org/10.1007/s00477-021-02113-x, 2022. a
Yang, S., Li, X., Zeng, L., Yu, X., Liu, Y., Lu, S., Huang, X., Zhang, D., Xu, H., Lin, S., Liu, H., Feng, M., Song, D., Tan, Q., Cui, J., Wang, L., Chen, Y., Wang, W., Sun, H., Song, M., Kong, L., Liu, Y., Wei, L., Zhu, X., and Zhang, Y.: Development of multi-channel whole-air sampling equipment onboard an unmanned aerial vehicle for investigating volatile organic compounds' vertical distribution in the planetary boundary layer, Atmos. Meas. Tech., 16, 501–512, https://doi.org/10.5194/amt-16-501-2023, 2023. a
Zhang, L., Brook, J. R., and Vet, R.: A revised parameterization for gaseous dry deposition in air-quality models, Atmos. Chem. Phys., 3, 2067–2082, https://doi.org/10.5194/acp-3-2067-2003, 2003. a
Short summary
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.
Four-dimensional variational data assimilation allows for the simultaneous optimisation of...
Altmetrics
Final-revised paper
Preprint