Articles | Volume 23, issue 19
https://doi.org/10.5194/acp-23-12631-2023
© Author(s) 2023. 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-23-12631-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
11 Oct 2023
Research article |
| 11 Oct 2023
| 11 Oct 2023
Atmospheric photooxidation and ozonolysis of sabinene: reaction rate coefficients, product yields, and chemical budget of radicals
Jacky Y. S. Pang
Institute of Energy and Climate Research, IEK-8: Troposphere,
Forschungszentrum Jülich GmbH, Jülich, Germany
Florian Berg
Institute of Energy and Climate Research, IEK-8: Troposphere,
Forschungszentrum Jülich GmbH, Jülich, Germany
Anna Novelli
Institute of Energy and Climate Research, IEK-8: Troposphere,
Forschungszentrum Jülich GmbH, Jülich, Germany
Birger Bohn
Institute of Energy and Climate Research, IEK-8: Troposphere,
Forschungszentrum Jülich GmbH, Jülich, Germany
Michelle Färber
Institute of Energy and Climate Research, IEK-8: Troposphere,
Forschungszentrum Jülich GmbH, Jülich, Germany
Philip T. M. Carlsson
Institute of Energy and Climate Research, IEK-8: Troposphere,
Forschungszentrum Jülich GmbH, Jülich, Germany
René Dubus
Institute of Energy and Climate Research, IEK-8: Troposphere,
Forschungszentrum Jülich GmbH, Jülich, Germany
Georgios I. Gkatzelis
Institute of Energy and Climate Research, IEK-8: Troposphere,
Forschungszentrum Jülich GmbH, Jülich, Germany
Franz Rohrer
Institute of Energy and Climate Research, IEK-8: Troposphere,
Forschungszentrum Jülich GmbH, Jülich, Germany
Sergej Wedel
Institute of Energy and Climate Research, IEK-8: Troposphere,
Forschungszentrum Jülich GmbH, Jülich, Germany
Andreas Wahner
Institute of Energy and Climate Research, IEK-8: Troposphere,
Forschungszentrum Jülich GmbH, Jülich, Germany
Institute of Energy and Climate Research, IEK-8: Troposphere,
Forschungszentrum Jülich GmbH, Jülich, Germany
Department of Physics, University of Cologne, Cologne, Germany
Related authors
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.
Biplob Dey, Toke Due Sjøgren, Peeyush Khare, Georgios I. Gkatzelis, Yizhen Wu, Sindhu Vasireddy, Martin Schultz, Alexander Knohl, Riikka Rinnan, Thorsten Hohaus, and Eva Y. Pfannerstill
EGUsphere, https://doi.org/10.5194/egusphere-2025-3779, https://doi.org/10.5194/egusphere-2025-3779, 2025
This preprint is open for discussion and under review for Biogeosciences (BG).
Short summary
Short summary
Trees release reactive gases that affect air quality and climate. We studied how these emissions from European beech and English oak change under realistic scenarios of combined and single heat and ozone stress. Heat increased emissions, while ozone reduced most of them. When stressors were combined, the effects were complex and varied by species. Machine learning identified key stress-related compounds. Our findings show that future tree stress may alter air quality and climate interactions.
Paolo Andreozzi, Mark D. Fielding, Robin J. Hogan, Richard M. Forbes, Samuel Rémy, Birger Bohn, and Ulrich Löhnert
EGUsphere, https://doi.org/10.5194/egusphere-2025-3790, https://doi.org/10.5194/egusphere-2025-3790, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
Short summary
Short summary
Aerosols significantly contribute to the Earth’s climate, but models still struggle at representing them. Here we use satellite observations of clouds to improve aerosols in our weather and air-quality model. We show that African wildfires induce too bright simulated clouds and that our model removes too much aerosol from ice-containing clouds. This showcases how our approach effectively targets poorly observed aerosol processes, potentially informing weather forecasting and climate models.
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
EGUsphere, https://doi.org/10.5194/egusphere-2025-3074, https://doi.org/10.5194/egusphere-2025-3074, 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.
Susanne M. C. Scholz, Vlassis A. Karydis, Georgios I. Gkatzelis, Hendrik Fuchs, Spyros N. Pandis, and Alexandra P. Tsimpidi
EGUsphere, https://doi.org/10.5194/egusphere-2025-2510, https://doi.org/10.5194/egusphere-2025-2510, 2025
Short summary
Short summary
We studied how pollution from cars and trucks contributes to tiny airborne particles that affect air quality and climate. These particles, called secondary organic aerosols, were often underestimated in global models. By improving how certain overlooked emissions from fuel use are represented in our model, we found that their impact is much larger than previously thought. Our results suggest that road traffic plays a far greater role in global air pollution than earlier estimates showed.
Sungah Kang, Jürgen Wildt, Iida Pullinen, Luc Vereecken, Cheng Wu, Andreas Wahner, Sören R. Zorn, and Thomas F. Mentel
EGUsphere, https://doi.org/10.5194/egusphere-2025-2772, https://doi.org/10.5194/egusphere-2025-2772, 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.
Alexander Hermanns, Anne Caroline Lange, Julia Kowalski, Hendrik Fuchs, and Philipp Franke
EGUsphere, https://doi.org/10.5194/egusphere-2025-450, https://doi.org/10.5194/egusphere-2025-450, 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 EURAD-IM.
Joseph O. Palmo, Colette L. Heald, Donald R. Blake, Ilann Bourgeois, Matthew Coggon, Jeff Collett, Frank Flocke, Alan Fried, Georgios Gkatzelis, Samuel Hall, Lu Hu, Jose L. Jimenez, Pedro Campuzano-Jost, I-Ting Ku, Benjamin Nault, Brett Palm, Jeff Peischl, Ilana Pollack, Amy Sullivan, Joel Thornton, Carsten Warneke, Armin Wisthaler, and Lu Xu
EGUsphere, https://doi.org/10.5194/egusphere-2025-1969, https://doi.org/10.5194/egusphere-2025-1969, 2025
Short summary
Short summary
This study investigates ozone production within wildfire smoke plumes as they age, using both aircraft observations and models. We find that the chemical environment and resulting ozone production within smoke changes as plumes evolve, with implications for climate and public health.
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.
Alexandros Milousis, Susanne M. C. Scholz, Hendrik Fuchs, Alexandra P. Tsimpidi, and Vlassis A. Karydis
EGUsphere, https://doi.org/10.5194/egusphere-2025-313, https://doi.org/10.5194/egusphere-2025-313, 2025
Short summary
Short summary
Nitrate aerosol has become a dominant atmospheric component, surpassing sulfate in aerosol composition. However, its simulation remains challenging due to complex formation processes and regional variability. We use the EMAC model to assess key factors in nitrate aerosol predictions. Increasing grid resolution, reducing N2O5 hydrolysis uptake, and refined emissions improve PM2.5 predictions, but PM1 remains underestimated. Seasonal & diurnal discrepancies persist, requiring further refinements.
Hassnae Erraji, Philipp Franke, Astrid Lampert, Tobias Schuldt, Ralf Tillmann, Andreas Wahner, and Anne Caroline Lange
Atmos. Chem. Phys., 24, 13913–13934, https://doi.org/10.5194/acp-24-13913-2024, https://doi.org/10.5194/acp-24-13913-2024, 2024
Short summary
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.
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.
Andrew O. Langford, Raul J. Alvarez II, Kenneth C. Aikin, Sunil Baidar, W. Alan Brewer, Steven S. Brown, Matthew M. Coggan, Patrick D. Cullis, Jessica Gilman, Georgios I. Gkatzelis, Detlev Helmig, Bryan J. Johnson, K. Emma Knowland, Rajesh Kumar, Aaron D. Lamplugh, Audra McClure-Begley, Brandi J. McCarty, Ann M. Middlebrook, Gabriele Pfister, Jeff Peischl, Irina Petropavlovskikh, Pamela S. Rickley, Andrew W. Rollins, Scott P. Sandberg, Christoph J. Senff, and Carsten Warneke
EGUsphere, https://doi.org/10.5194/egusphere-2024-1938, https://doi.org/10.5194/egusphere-2024-1938, 2024
Preprint withdrawn
Short summary
Short summary
High ozone (O3) formed by reactions of nitrogen oxides (NOx) and volatile organic compounds (VOCs) can harm human health and welfare. High O3 is usually associated with hot summer days, but under certain conditions, high O3 can also form under winter conditions. In this study, we describe a high O3 event that occurred in Colorado during the COVID-19 quarantine that was caused in part by the decrease in traffic, and in part by a shallow inversion created by descent of stratospheric air.
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
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.
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.
Matthew M. Coggon, Chelsea E. Stockwell, Megan S. Claflin, Eva Y. Pfannerstill, Lu Xu, Jessica B. Gilman, Julia Marcantonio, Cong Cao, Kelvin Bates, Georgios I. Gkatzelis, Aaron Lamplugh, Erin F. Katz, Caleb Arata, Eric C. Apel, Rebecca S. Hornbrook, Felix Piel, Francesca Majluf, Donald R. Blake, Armin Wisthaler, Manjula Canagaratna, Brian M. Lerner, Allen H. Goldstein, John E. Mak, and Carsten Warneke
Atmos. Meas. Tech., 17, 801–825, https://doi.org/10.5194/amt-17-801-2024, https://doi.org/10.5194/amt-17-801-2024, 2024
Short summary
Short summary
Mass spectrometry is a tool commonly used to measure air pollutants. This study evaluates measurement artifacts produced in the proton-transfer-reaction mass spectrometer. We provide methods to correct these biases and better measure compounds that degrade air quality.
Georgios I. Gkatzelis, Matthew M. Coggon, Chelsea E. Stockwell, Rebecca S. Hornbrook, Hannah Allen, Eric C. Apel, Megan M. Bela, Donald R. Blake, Ilann Bourgeois, Steven S. Brown, Pedro Campuzano-Jost, Jason M. St. Clair, James H. Crawford, John D. Crounse, Douglas A. Day, Joshua P. DiGangi, Glenn S. Diskin, Alan Fried, Jessica B. Gilman, Hongyu Guo, Johnathan W. Hair, Hannah S. Halliday, Thomas F. Hanisco, Reem Hannun, Alan Hills, L. Gregory Huey, Jose L. Jimenez, Joseph M. Katich, Aaron Lamplugh, Young Ro Lee, Jin Liao, Jakob Lindaas, Stuart A. McKeen, Tomas Mikoviny, Benjamin A. Nault, J. Andrew Neuman, John B. Nowak, Demetrios Pagonis, Jeff Peischl, Anne E. Perring, Felix Piel, Pamela S. Rickly, Michael A. Robinson, Andrew W. Rollins, Thomas B. Ryerson, Melinda K. Schueneman, Rebecca H. Schwantes, Joshua P. Schwarz, Kanako Sekimoto, Vanessa Selimovic, Taylor Shingler, David J. Tanner, Laura Tomsche, Krystal T. Vasquez, Patrick R. Veres, Rebecca Washenfelder, Petter Weibring, Paul O. Wennberg, Armin Wisthaler, Glenn M. Wolfe, Caroline C. Womack, Lu Xu, Katherine Ball, Robert J. Yokelson, and Carsten Warneke
Atmos. Chem. Phys., 24, 929–956, https://doi.org/10.5194/acp-24-929-2024, https://doi.org/10.5194/acp-24-929-2024, 2024
Short summary
Short summary
This study reports emissions of gases and particles from wildfires. These emissions are related to chemical proxies that can be measured by satellite and incorporated into models to improve predictions of wildfire impacts on air quality and climate.
Marc von Hobe, Domenico Taraborrelli, Sascha Alber, Birger Bohn, Hans-Peter Dorn, Hendrik Fuchs, Yun Li, Chenxi Qiu, Franz Rohrer, Roberto Sommariva, Fred Stroh, Zhaofeng Tan, Sergej Wedel, and Anna Novelli
Atmos. Chem. Phys., 23, 10609–10623, https://doi.org/10.5194/acp-23-10609-2023, https://doi.org/10.5194/acp-23-10609-2023, 2023
Short summary
Short summary
The trace gas carbonyl sulfide (OCS) transports sulfur from the troposphere to the stratosphere, where sulfate aerosols are formed that influence climate and stratospheric chemistry. An uncertain OCS source in the troposphere is chemical production form dimethyl sulfide (DMS), a gas released in large quantities from the oceans. We carried out experiments in a large atmospheric simulation chamber to further elucidate the chemical mechanism of OCS production from DMS.
Midhun George, Maria Dolores Andrés Hernández, Vladyslav Nenakhov, Yangzhuoran Liu, John Philip Burrows, Birger Bohn, Eric Förster, Florian Obersteiner, Andreas Zahn, Theresa Harlaß, Helmut Ziereis, Hans Schlager, Benjamin Schreiner, Flora Kluge, Katja Bigge, and Klaus Pfeilsticker
Atmos. Chem. Phys., 23, 7799–7822, https://doi.org/10.5194/acp-23-7799-2023, https://doi.org/10.5194/acp-23-7799-2023, 2023
Short summary
Short summary
The applicability of photostationary steady-state (PSS) assumptions to estimate the amount of the sum of peroxy radicals (RO2*) during the EMeRGe airborne observations from the known radical chemistry and onboard measurements of RO2* precursors, photolysis frequencies, and other trace gases such as NOx and O3 was investigated. The comparison of the calculated RO2* with the actual measurements provides an insight into the main processes controlling their concentration in the air masses measured.
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.
Lixu Jin, Wade Permar, Vanessa Selimovic, Damien Ketcherside, Robert J. Yokelson, Rebecca S. Hornbrook, Eric C. Apel, I-Ting Ku, Jeffrey L. Collett Jr., Amy P. Sullivan, Daniel A. Jaffe, Jeffrey R. Pierce, Alan Fried, Matthew M. Coggon, Georgios I. Gkatzelis, Carsten Warneke, Emily V. Fischer, and Lu Hu
Atmos. Chem. Phys., 23, 5969–5991, https://doi.org/10.5194/acp-23-5969-2023, https://doi.org/10.5194/acp-23-5969-2023, 2023
Short summary
Short summary
Air quality in the USA has been improving since 1970 due to anthropogenic emission reduction. Those gains have been partly offset by increased wildfire pollution in the western USA in the past 20 years. Still, we do not understand wildfire emissions well due to limited measurements. Here, we used a global transport model to evaluate and constrain current knowledge of wildfire emissions with recent observational constraints, showing the underestimation of wildfire emissions in the western USA.
Zaneta Hamryszczak, Dirk Dienhart, Bettina Brendel, Roland Rohloff, Daniel Marno, Monica Martinez, Hartwig Harder, Andrea Pozzer, Birger Bohn, Martin Zöger, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 23, 5929–5943, https://doi.org/10.5194/acp-23-5929-2023, https://doi.org/10.5194/acp-23-5929-2023, 2023
Short summary
Short summary
Hydrogen peroxide is a key contributor to the oxidative chemistry of the atmosphere through its link to the most prominent oxidants controlling its self-cleansing capacity, HOx. During the CAFE-Africa campaign, H2O2 was measured over the Atlantic Ocean and western Africa in August/September 2018. The study gives an overview of the distribution of H2O2 in the upper tropical troposphere and investigates the impact of convective processes in the Intertropical Convergence Zone on the budget of H2O2.
Kezia Lange, Andreas Richter, Anja Schönhardt, Andreas C. Meier, Tim Bösch, André Seyler, Kai Krause, Lisa K. Behrens, Folkard Wittrock, Alexis Merlaud, Frederik Tack, Caroline Fayt, Martina M. Friedrich, Ermioni Dimitropoulou, Michel Van Roozendael, Vinod Kumar, Sebastian Donner, Steffen Dörner, Bianca Lauster, Maria Razi, Christian Borger, Katharina Uhlmannsiek, Thomas Wagner, Thomas Ruhtz, Henk Eskes, Birger Bohn, Daniel Santana Diaz, Nader Abuhassan, Dirk Schüttemeyer, and John P. Burrows
Atmos. Meas. Tech., 16, 1357–1389, https://doi.org/10.5194/amt-16-1357-2023, https://doi.org/10.5194/amt-16-1357-2023, 2023
Short summary
Short summary
We present airborne imaging DOAS and ground-based stationary and car DOAS measurements conducted during the S5P-VAL-DE-Ruhr campaign in the Rhine-Ruhr region. The measurements are used to validate spaceborne NO2 data products from the Sentinel-5 Precursor TROPOspheric Monitoring Instrument (TROPOMI). Auxiliary data of the TROPOMI NO2 retrieval, such as spatially higher resolved a priori NO2 vertical profiles, surface reflectivity, and cloud treatment are investigated to evaluate their impact.
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.
Chuan-Yao Lin, Wan-Chin Chen, Yi-Yun Chien, Charles C. K. Chou, Chian-Yi Liu, Helmut Ziereis, Hans Schlager, Eric Förster, Florian Obersteiner, Ovid O. Krüger, Bruna A. Holanda, Mira L. Pöhlker, Katharina Kaiser, Johannes Schneider, Birger Bohn, Klaus Pfeilsticker, Benjamin Weyland, Maria Dolores Andrés Hernández, and John P. Burrows
Atmos. Chem. Phys., 23, 2627–2647, https://doi.org/10.5194/acp-23-2627-2023, https://doi.org/10.5194/acp-23-2627-2023, 2023
Short summary
Short summary
During the EMeRGe campaign in Asia, atmospheric pollutants were measured on board the HALO aircraft. The WRF-Chem model was employed to evaluate the biomass burning (BB) plume transported from Indochina and its impact on the downstream areas. The combination of BB aerosol enhancement with cloud water resulted in a reduction in incoming shortwave radiation at the surface in southern China and the East China Sea, which potentially has significant regional climate implications.
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).
Birger Bohn and Insa Lohse
Atmos. Meas. Tech., 16, 209–233, https://doi.org/10.5194/amt-16-209-2023, https://doi.org/10.5194/amt-16-209-2023, 2023
Short summary
Short summary
Optical receivers for solar spectral actinic radiation are designed for angle-independent sensitivities within a hemisphere. Remaining imperfections can be compensated for by receiver-specific corrections based on laboratory characterizations and radiative transfer calculations of spectral radiance distributions. The corrections cover a wide range of realistic atmospheric conditions and were applied to ground-based and airborne measurements in a wavelength range 280–660 nm.
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.
Therese S. Carter, Colette L. Heald, Jesse H. Kroll, Eric C. Apel, Donald Blake, Matthew Coggon, Achim Edtbauer, Georgios Gkatzelis, Rebecca S. Hornbrook, Jeff Peischl, Eva Y. Pfannerstill, Felix Piel, Nina G. Reijrink, Akima Ringsdorf, Carsten Warneke, Jonathan Williams, Armin Wisthaler, and Lu Xu
Atmos. Chem. Phys., 22, 12093–12111, https://doi.org/10.5194/acp-22-12093-2022, https://doi.org/10.5194/acp-22-12093-2022, 2022
Short summary
Short summary
Fires emit many gases which can contribute to smog and air pollution. However, the amount and properties of these chemicals are not well understood, so this work updates and expands their representation in a global atmospheric model, including by adding new chemicals. We confirm that this updated representation generally matches measurements taken in several fire regions. We then show that fires provide ~15 % of atmospheric reactivity globally and more than 75 % over fire source regions.
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.
Ilann Bourgeois, Jeff Peischl, J. Andrew Neuman, Steven S. Brown, Hannah M. Allen, Pedro Campuzano-Jost, Matthew M. Coggon, Joshua P. DiGangi, Glenn S. Diskin, Jessica B. Gilman, Georgios I. Gkatzelis, Hongyu Guo, Hannah A. Halliday, Thomas F. Hanisco, Christopher D. Holmes, L. Gregory Huey, Jose L. Jimenez, Aaron D. Lamplugh, Young Ro Lee, Jakob Lindaas, Richard H. Moore, Benjamin A. Nault, John B. Nowak, Demetrios Pagonis, Pamela S. Rickly, Michael A. Robinson, Andrew W. Rollins, Vanessa Selimovic, Jason M. St. Clair, David Tanner, Krystal T. Vasquez, Patrick R. Veres, Carsten Warneke, Paul O. Wennberg, Rebecca A. Washenfelder, Elizabeth B. Wiggins, Caroline C. Womack, Lu Xu, Kyle J. Zarzana, and Thomas B. Ryerson
Atmos. Meas. Tech., 15, 4901–4930, https://doi.org/10.5194/amt-15-4901-2022, https://doi.org/10.5194/amt-15-4901-2022, 2022
Short summary
Short summary
Understanding fire emission impacts on the atmosphere is key to effective air quality management and requires accurate measurements. We present a comparison of airborne measurements of key atmospheric species in ambient air and in fire smoke. We show that most instruments performed within instrument uncertainties. In some cases, further work is needed to fully characterize instrument performance. Comparing independent measurements using different techniques is important to assess their accuracy.
Shang Liu, Barbara Barletta, Rebecca S. Hornbrook, Alan Fried, Jeff Peischl, Simone Meinardi, Matthew Coggon, Aaron Lamplugh, Jessica B. Gilman, Georgios I. Gkatzelis, Carsten Warneke, Eric C. Apel, Alan J. Hills, Ilann Bourgeois, James Walega, Petter Weibring, Dirk Richter, Toshihiro Kuwayama, Michael FitzGibbon, and Donald Blake
Atmos. Chem. Phys., 22, 10937–10954, https://doi.org/10.5194/acp-22-10937-2022, https://doi.org/10.5194/acp-22-10937-2022, 2022
Short summary
Short summary
California’s ozone persistently exceeds the air quality standards. We studied the spatial distribution of volatile organic compounds (VOCs) that produce ozone over the most polluted regions in California using aircraft measurements. We find that the oxygenated VOCs have the highest ozone formation potential. Spatially, biogenic VOCs are important during high ozone episodes in the South Coast Air Basin, while dairy emissions may be critical for ozone production in San Joaquin Valley.
Simon F. Reifenberg, Anna Martin, Matthias Kohl, Sara Bacer, Zaneta Hamryszczak, Ivan Tadic, Lenard Röder, Daniel J. Crowley, Horst Fischer, Katharina Kaiser, Johannes Schneider, Raphael Dörich, John N. Crowley, Laura Tomsche, Andreas Marsing, Christiane Voigt, Andreas Zahn, Christopher Pöhlker, Bruna A. Holanda, Ovid Krüger, Ulrich Pöschl, Mira Pöhlker, Patrick Jöckel, Marcel Dorf, Ulrich Schumann, Jonathan Williams, Birger Bohn, Joachim Curtius, Hardwig Harder, Hans Schlager, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 22, 10901–10917, https://doi.org/10.5194/acp-22-10901-2022, https://doi.org/10.5194/acp-22-10901-2022, 2022
Short summary
Short summary
In this work we use a combination of observational data from an aircraft campaign and model results to investigate the effect of the European lockdown due to COVID-19 in spring 2020. Using model results, we show that the largest relative changes to the atmospheric composition caused by the reduced emissions are located in the upper troposphere around aircraft cruise altitude, while the largest absolute changes are present at the surface.
Zaneta T. Hamryszczak, Andrea Pozzer, Florian Obersteiner, Birger Bohn, Benedikt Steil, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 22, 9483–9497, https://doi.org/10.5194/acp-22-9483-2022, https://doi.org/10.5194/acp-22-9483-2022, 2022
Short summary
Short summary
Hydrogen peroxide plays a pivotal role in the chemistry of the atmosphere. Together with organic hydroperoxides, it forms a reservoir for peroxy radicals, which are known to be the key contributors to the self-cleaning processes of the atmosphere. Hydroperoxides were measured over Europe during the BLUESKY campaign in May–June 2020. The paper gives an overview of the distribution of the species in the troposphere and investigates the impact of wet scavenging and deposition on the budget of H2O2.
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.
M. Dolores Andrés Hernández, Andreas Hilboll, Helmut Ziereis, Eric Förster, Ovid O. Krüger, Katharina Kaiser, Johannes Schneider, Francesca Barnaba, Mihalis Vrekoussis, Jörg Schmidt, Heidi Huntrieser, Anne-Marlene Blechschmidt, Midhun George, Vladyslav Nenakhov, Theresa Harlass, Bruna A. Holanda, Jennifer Wolf, Lisa Eirenschmalz, Marc Krebsbach, Mira L. Pöhlker, Anna B. Kalisz Hedegaard, Linlu Mei, Klaus Pfeilsticker, Yangzhuoran Liu, Ralf Koppmann, Hans Schlager, Birger Bohn, Ulrich Schumann, Andreas Richter, Benjamin Schreiner, Daniel Sauer, Robert Baumann, Mariano Mertens, Patrick Jöckel, Markus Kilian, Greta Stratmann, Christopher Pöhlker, Monica Campanelli, Marco Pandolfi, Michael Sicard, José L. Gómez-Amo, Manuel Pujadas, Katja Bigge, Flora Kluge, Anja Schwarz, Nikos Daskalakis, David Walter, Andreas Zahn, Ulrich Pöschl, Harald Bönisch, Stephan Borrmann, Ulrich Platt, and John P. Burrows
Atmos. Chem. Phys., 22, 5877–5924, https://doi.org/10.5194/acp-22-5877-2022, https://doi.org/10.5194/acp-22-5877-2022, 2022
Short summary
Short summary
EMeRGe provides a unique set of in situ and remote sensing airborne measurements of trace gases and aerosol particles along selected flight routes in the lower troposphere over Europe. The interpretation uses also complementary collocated ground-based and satellite measurements. The collected data help to improve the current understanding of the complex spatial distribution of trace gases and aerosol particles resulting from mixing, transport, and transformation of pollution plumes over Europe.
Sophie Dixneuf, Albert A. Ruth, Rolf Häseler, Theo Brauers, Franz Rohrer, and Hans-Peter Dorn
Atmos. Meas. Tech., 15, 945–964, https://doi.org/10.5194/amt-15-945-2022, https://doi.org/10.5194/amt-15-945-2022, 2022
Short summary
Short summary
Atmospheric chambers, like SAPHIR in Jülich (Germany), are used to experimentally simulate specific atmospheric scenarios to improve our understanding of the complex chemical reactions occurring in our atmospheres. These facilities hence require cutting-edge gas-sensing capabilities to detect trace gases at the lowest level and in a short time. One important trace gas is HONO, for which we custom-built an optical sensing setup, capable of detecting one HONO molecule in ~40 billion in 1 min.
Jin Liao, Glenn M. Wolfe, Reem A. Hannun, Jason M. St. Clair, Thomas F. Hanisco, Jessica B. Gilman, Aaron Lamplugh, Vanessa Selimovic, Glenn S. Diskin, John B. Nowak, Hannah S. Halliday, Joshua P. DiGangi, Samuel R. Hall, Kirk Ullmann, Christopher D. Holmes, Charles H. Fite, Anxhelo Agastra, Thomas B. Ryerson, Jeff Peischl, Ilann Bourgeois, Carsten Warneke, Matthew M. Coggon, Georgios I. Gkatzelis, Kanako Sekimoto, Alan Fried, Dirk Richter, Petter Weibring, Eric C. Apel, Rebecca S. Hornbrook, Steven S. Brown, Caroline C. Womack, Michael A. Robinson, Rebecca A. Washenfelder, Patrick R. Veres, and J. Andrew Neuman
Atmos. Chem. Phys., 21, 18319–18331, https://doi.org/10.5194/acp-21-18319-2021, https://doi.org/10.5194/acp-21-18319-2021, 2021
Short summary
Short summary
Formaldehyde (HCHO) is an important oxidant precursor and affects the formation of O3 and other secondary pollutants in wildfire plumes. We disentangle the processes controlling HCHO evolution from wildfire plumes sampled by NASA DC-8 during FIREX-AQ. We find that OH abundance rather than normalized OH reactivity is the main driver of fire-to-fire variability in HCHO secondary production and estimate an effective HCHO yield per volatile organic compound molecule oxidized in wildfire plumes.
Clara M. Nussbaumer, John N. Crowley, Jan Schuladen, Jonathan Williams, Sascha Hafermann, Andreas Reiffs, Raoul Axinte, Hartwig Harder, Cheryl Ernest, Anna Novelli, Katrin Sala, Monica Martinez, Chinmay Mallik, Laura Tomsche, Christian Plass-Dülmer, Birger Bohn, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 18413–18432, https://doi.org/10.5194/acp-21-18413-2021, https://doi.org/10.5194/acp-21-18413-2021, 2021
Short summary
Short summary
HCHO is an important atmospheric trace gas influencing the photochemical processes in the Earth’s atmosphere, including the budget of HOx and the abundance of tropospheric O3. This research presents the photochemical calculations of HCHO and O3 based on three field campaigns across Europe. We show that HCHO production via the oxidation of only four volatile organic compound precursors, i.e., CH4, CH3CHO, C5H8 and CH3OH, can balance the observed loss at all sites well.
Zachary C. J. Decker, Michael A. Robinson, Kelley C. Barsanti, Ilann Bourgeois, Matthew M. Coggon, Joshua P. DiGangi, Glenn S. Diskin, Frank M. Flocke, Alessandro Franchin, Carley D. Fredrickson, Georgios I. Gkatzelis, Samuel R. Hall, Hannah Halliday, Christopher D. Holmes, L. Gregory Huey, Young Ro Lee, Jakob Lindaas, Ann M. Middlebrook, Denise D. Montzka, Richard Moore, J. Andrew Neuman, John B. Nowak, Brett B. Palm, Jeff Peischl, Felix Piel, Pamela S. Rickly, Andrew W. Rollins, Thomas B. Ryerson, Rebecca H. Schwantes, Kanako Sekimoto, Lee Thornhill, Joel A. Thornton, Geoffrey S. Tyndall, Kirk Ullmann, Paul Van Rooy, Patrick R. Veres, Carsten Warneke, Rebecca A. Washenfelder, Andrew J. Weinheimer, Elizabeth Wiggins, Edward Winstead, Armin Wisthaler, Caroline Womack, and Steven S. Brown
Atmos. Chem. Phys., 21, 16293–16317, https://doi.org/10.5194/acp-21-16293-2021, https://doi.org/10.5194/acp-21-16293-2021, 2021
Short summary
Short summary
To understand air quality impacts from wildfires, we need an accurate picture of how wildfire smoke changes chemically both day and night as sunlight changes the chemistry of smoke. We present a chemical analysis of wildfire smoke as it changes from midday through the night. We use aircraft observations from the FIREX-AQ field campaign with a chemical box model. We find that even under sunlight typical
nighttimechemistry thrives and controls the fate of key smoke plume chemical processes.
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.
Clara M. Nussbaumer, Uwe Parchatka, Ivan Tadic, Birger Bohn, Daniel Marno, Monica Martinez, Roland Rohloff, Hartwig Harder, Flora Kluge, Klaus Pfeilsticker, Florian Obersteiner, Martin Zöger, Raphael Doerich, John N. Crowley, Jos Lelieveld, and Horst Fischer
Atmos. Meas. Tech., 14, 6759–6776, https://doi.org/10.5194/amt-14-6759-2021, https://doi.org/10.5194/amt-14-6759-2021, 2021
Short summary
Short summary
NO2 plays a central role in atmospheric photochemical processes and requires accurate measurements. This research presents NO2 data obtained via chemiluminescence using a photolytic converter from airborne studies around Cabo Verde and laboratory investigations. We show the limits and error-proneness of a conventional blue light converter in aircraft measurements affected by humidity and NO levels and suggest the use of an alternative quartz converter for more reliable results.
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.
Benjamin A. Nault, Duseong S. Jo, Brian C. McDonald, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Jason C. Schroder, James Allan, Donald R. Blake, Manjula R. Canagaratna, Hugh Coe, Matthew M. Coggon, Peter F. DeCarlo, Glenn S. Diskin, Rachel Dunmore, Frank Flocke, Alan Fried, Jessica B. Gilman, Georgios Gkatzelis, Jacqui F. Hamilton, Thomas F. Hanisco, Patrick L. Hayes, Daven K. Henze, Alma Hodzic, James Hopkins, Min Hu, L. Greggory Huey, B. Thomas Jobson, William C. Kuster, Alastair Lewis, Meng Li, Jin Liao, M. Omar Nawaz, Ilana B. Pollack, Jeffrey Peischl, Bernhard Rappenglück, Claire E. Reeves, Dirk Richter, James M. Roberts, Thomas B. Ryerson, Min Shao, Jacob M. Sommers, James Walega, Carsten Warneke, Petter Weibring, Glenn M. Wolfe, Dominique E. Young, Bin Yuan, Qiang Zhang, Joost A. de Gouw, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 11201–11224, https://doi.org/10.5194/acp-21-11201-2021, https://doi.org/10.5194/acp-21-11201-2021, 2021
Short summary
Short summary
Secondary organic aerosol (SOA) is an important aspect of poor air quality for urban regions around the world, where a large fraction of the population lives. However, there is still large uncertainty in predicting SOA in urban regions. Here, we used data from 11 urban campaigns and show that the variability in SOA production in these regions is predictable and is explained by key emissions. These results are used to estimate the premature mortality associated with SOA in urban regions.
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.
Ivan Tadic, Clara M. Nussbaumer, Birger Bohn, Hartwig Harder, Daniel Marno, Monica Martinez, Florian Obersteiner, Uwe Parchatka, Andrea Pozzer, Roland Rohloff, Martin Zöger, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 8195–8211, https://doi.org/10.5194/acp-21-8195-2021, https://doi.org/10.5194/acp-21-8195-2021, 2021
Short summary
Short summary
Although mechanisms of tropospheric ozone (O3) formation are well understood, studies reporting on ozone formation derived from field measurements are challenging and remain sparse in number. We use airborne measurements to quantify nitric oxide (NO) and O3 distributions in the upper troposphere over the Atlantic Ocean and western Africa and compare our measurements to model simulations. Our results show that NO and ozone formation are greatest over the tropical areas of western Africa.
Chelsea E. Stockwell, Matthew M. Coggon, Georgios I. Gkatzelis, John Ortega, Brian C. McDonald, Jeff Peischl, Kenneth Aikin, Jessica B. Gilman, Michael Trainer, and Carsten Warneke
Atmos. Chem. Phys., 21, 6005–6022, https://doi.org/10.5194/acp-21-6005-2021, https://doi.org/10.5194/acp-21-6005-2021, 2021
Short summary
Short summary
Volatile chemical products are emerging as a large source of petrochemical organics in urban environments. We identify markers for the coatings category by linking ambient observations to laboratory measurements, investigating volatile organic compound (VOC) composition, and quantifying key VOC emissions via controlled evaporation experiments. Ingredients and sales surveys are used to confirm the prevalence and usage trends to support the assignment of water and solvent-borne coating tracers.
Alexander Zaytsev, Martin Breitenlechner, Anna Novelli, Hendrik Fuchs, Daniel A. Knopf, Jesse H. Kroll, and Frank N. Keutsch
Atmos. Meas. Tech., 14, 2501–2513, https://doi.org/10.5194/amt-14-2501-2021, https://doi.org/10.5194/amt-14-2501-2021, 2021
Short summary
Short summary
We have developed an online method for speciated measurements of organic peroxy radicals and stabilized Criegee intermediates using chemical derivatization combined with chemical ionization mass spectrometry. Chemical derivatization prevents secondary radical reactions and eliminates potential interferences. Comparison between our measurements and results from numeric modeling shows that the method can be used for the quantification of a wide range of atmospheric radicals and intermediates.
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.
Demetrios Pagonis, Pedro Campuzano-Jost, Hongyu Guo, Douglas A. Day, Melinda K. Schueneman, Wyatt L. Brown, Benjamin A. Nault, Harald Stark, Kyla Siemens, Alex Laskin, Felix Piel, Laura Tomsche, Armin Wisthaler, Matthew M. Coggon, Georgios I. Gkatzelis, Hannah S. Halliday, Jordan E. Krechmer, Richard H. Moore, David S. Thomson, Carsten Warneke, Elizabeth B. Wiggins, and Jose L. Jimenez
Atmos. Meas. Tech., 14, 1545–1559, https://doi.org/10.5194/amt-14-1545-2021, https://doi.org/10.5194/amt-14-1545-2021, 2021
Short summary
Short summary
We describe the airborne deployment of an extractive electrospray time-of-flight mass spectrometer (EESI-MS). The instrument provides a quantitative 1 Hz measurement of the chemical composition of organic aerosol up to altitudes of
7 km, with single-compound detection limits as low as 50 ng per standard cubic meter.
Huan Song, Xiaorui Chen, Keding Lu, Qi Zou, Zhaofeng Tan, Hendrik Fuchs, Alfred Wiedensohler, Daniel R. Moon, Dwayne E. Heard, María-Teresa Baeza-Romero, Mei Zheng, Andreas Wahner, Astrid Kiendler-Scharr, and Yuanhang Zhang
Atmos. Chem. Phys., 20, 15835–15850, https://doi.org/10.5194/acp-20-15835-2020, https://doi.org/10.5194/acp-20-15835-2020, 2020
Short summary
Short summary
Accurate calculation of the HO2 uptake coefficient is one of the key parameters to quantify the co-reduction of both aerosol and ozone pollution. We modelled various lab measurements of γHO2 based on a gas-liquid phase kinetic model and developed a state-of-the-art parameterized equation. Based on a dataset from a comprehensive field campaign in the North China Plain, we proposed that the determination of the heterogeneous uptake process for HO2 should be included in future field campaigns.
Michael Rolletter, Marion Blocquet, Martin Kaminski, Birger Bohn, Hans-Peter Dorn, Andreas Hofzumahaus, Frank Holland, Xin Li, Franz Rohrer, Ralf Tillmann, Robert Wegener, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 20, 13701–13719, https://doi.org/10.5194/acp-20-13701-2020, https://doi.org/10.5194/acp-20-13701-2020, 2020
Short summary
Short summary
The photooxidation of pinonaldehyde is investigated in a chamber study under natural sunlight and low NO conditions with and without an added hydroxyl radical (OH) scavenger. The experimentally determined pinonaldehyde photolysis frequency is faster by a factor of 3.5 than currently used parameterizations in atmospheric models. Yields of degradation products are measured in the presence and absence of OH. Measurements are compared to current atmospheric models and a theory-based mechanism.
Bettina Hottmann, Sascha Hafermann, Laura Tomsche, Daniel Marno, Monica Martinez, Hartwig Harder, Andrea Pozzer, Marco Neumaier, Andreas Zahn, Birger Bohn, Greta Stratmann, Helmut Ziereis, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 20, 12655–12673, https://doi.org/10.5194/acp-20-12655-2020, https://doi.org/10.5194/acp-20-12655-2020, 2020
Short summary
Short summary
During OMO we observed enhanced mixing ratios of hydroperoxides (ROOH) in the Asian monsoon anticyclone (AMA) relative to the background. The observed mixing ratios are higher than steady-state calculations and EMAC simulations, especially in the AMA, indicating atmospheric transport of ROOH. Uncertainties in the scavenging efficiencies likely cause deviations from EMAC. Longitudinal gradients indicate a pool of ROOH towards the center of the AMA associated with upwind convection over India.
Patrick Dewald, Jonathan M. Liebmann, Nils Friedrich, Justin Shenolikar, Jan Schuladen, Franz Rohrer, David Reimer, Ralf Tillmann, Anna Novelli, Changmin Cho, Kangming Xu, Rupert Holzinger, François Bernard, Li Zhou, Wahid Mellouki, Steven S. Brown, Hendrik Fuchs, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 10459–10475, https://doi.org/10.5194/acp-20-10459-2020, https://doi.org/10.5194/acp-20-10459-2020, 2020
Short summary
Short summary
We present direct measurements of NO3 reactivity resulting from the oxidation of isoprene by NO3 during an intensive simulation chamber study. Measurements were in excellent agreement with values calculated from measured isoprene amounts and the rate coefficient for the reaction of NO3 with isoprene. Comparison of the measurement with NO3 reactivities from non-steady-state and model calculations suggests that isoprene-derived RO2 and HO2 radicals account to ~ 50 % of overall NO3 losses.
Iida Pullinen, Sebastian Schmitt, Sungah Kang, Mehrnaz Sarrafzadeh, Patrick Schlag, Stefanie Andres, Einhard Kleist, Thomas F. Mentel, Franz Rohrer, Monika Springer, Ralf Tillmann, Jürgen Wildt, Cheng Wu, Defeng Zhao, Andreas Wahner, and Astrid Kiendler-Scharr
Atmos. Chem. Phys., 20, 10125–10147, https://doi.org/10.5194/acp-20-10125-2020, https://doi.org/10.5194/acp-20-10125-2020, 2020
Short summary
Short summary
Biogenic and anthropogenic air masses mix in the atmosphere, bringing plant-emitted monoterpenes and traffic-related nitrogen oxides together. There is debate whether the presence of nitrogen oxides reduces or increases secondary aerosol formation. This is important as secondary aerosols have cooling effects in the climate system but also constitute a health risk in populated areas. We show that the presence of NOx alone should not much affect the mass yields of secondary organic aerosols.
Cited articles
Almatarneh, M. H., Elayan, I. A., Altarawneh, M., and Hollett, J. W.: A
computational study of the ozonolysis of sabinene, Theor. Chem. Acc., 138,
30, https://doi.org/10.1007/s00214-019-2420-7, 2019.
Alvarado, A., Arey, J., and Atkinson, R.: Kinetics of the Gas-Phase
Reactions of OH and NO3 Radicals and O3 with the Monoterpene Reaction
Products Pinonaldehyde, Caronaldehyde, and Sabinaketone, J. Atmos. Chem.,
31, 281–297, https://doi.org/10.1023/A:1006010915971, 1998.
Arey, J., Atkinson, R., and Aschmann, S. M.: Product study of the gas-phase
reactions of monoterpenes with the OH radical in the presence of NO x,
J. Geophys. Res.-Atmos., 95, 18539–18546,
https://doi.org/10.1029/JD095iD11p18539, 1990.
Aschmann, S. M., Arey, J., and Atkinson, R.: OH radical formation from the
gas-phase reactions of O3 with a series of terpenes, Atmos. Environ., 36,
4347–4355, https://doi.org/10.1016/S1352-2310(02)00355-2, 2002.
Atkinson, R. and Arey, J.: Gas-phase tropospheric chemistry of biogenic
volatile organic compounds: a review, Atmos. Environ., 37, 197–219,
https://doi.org/10.1016/S1352-2310(03)00391-1, 2003.
Atkinson, R., Hasegawa, D., and Aschmann, S. M.: Rate constants for the gas-phase reactions of O3 with a series of monoterpenes and related compounds at 296 ± 2 K, Int. J. Chem.
Kinet., 22, 871–887, https://doi.org/10.1002/kin.550220807, 1990a.
Atkinson, R., Aschmann, S. M., and Arey, J.: Rate constants for the
gas-phase reactions of OH and NO3 radicals and O3 with sabinene and camphene
at 296 ± 2 K, Atmos. Environ., 24, 2647–2654,
https://doi.org/10.1016/0960-1686(90)90144-C, 1990b.
Atkinson, R., Aschmann, S. M., Arey, J., and Shorees, B.: Formation of OH
radicals in the gas phase reactions of O3 with a series of terpenes, J.
Geophys. Res., 97, 6065, https://doi.org/10.1029/92JD00062, 1992.
Atkinson, R., Baulch, D. L., Cox, R. A., Crowley, J. N., Hampson, R. F., Hynes, R. G., Jenkin, M. E., Rossi, M. J., and Troe, J.: Evaluated kinetic and photochemical data for atmospheric chemistry: Volume I - gas phase reactions of Ox, HOx, NOx and SOx species, Atmos. Chem. Phys., 4, 1461–1738, https://doi.org/10.5194/acp-4-1461-2004, 2004.
Atkinson, R., Baulch, D. L., Cox, R. A., Crowley, J. N., Hampson, R. F.,
Hynes, R. G., Jenkin, M. E., Rossi, M. J., Troe, J., and IUPAC Subcommittee:
Evaluated kinetic and photochemical data for atmospheric chemistry: Volume
II – gas phase reactions of organic species, Atmos. Chem. Phys., 6,
3625–4055, https://doi.org/10.5194/acp-6-3625-2006, 2006.
Barber, V. P., Pandit, S., Green, A. M., Trongsiriwat, N., Walsh, P. J.,
Klippenstein, S. J., and Lester, M. I.: Four-Carbon Criegee Intermediate
from Isoprene Ozonolysis: Methyl Vinyl Ketone Oxide Synthesis, Infrared
Spectrum, and OH Production, J. Am. Chem. Soc., 140, 10866–10880,
https://doi.org/10.1021/jacs.8b06010, 2018.
Bernard, F., Fedioun, I., Peyroux, F., Quilgars, A., Daële, V., and
Mellouki, A.: Thresholds of secondary organic aerosol formation by
ozonolysis of monoterpenes measured in a laminar flow aerosol reactor, J.
Aerosol Sci., 43, 14–30, https://doi.org/10.1016/j.jaerosci.2011.08.005,
2012.
Bohn, B. and Zilken, H.: Model-aided radiometric determination of photolysis frequencies in a sunlit atmosphere simulation chamber, Atmos. Chem. Phys., 5, 191–206, https://doi.org/10.5194/acp-5-191-2005, 2005.
Bohn, B., Rohrer, F., Brauers, T., and Wahner, A.: Actinometric measurements of NO2 photolysis frequencies in the atmosphere simulation chamber SAPHIR, Atmos. Chem. Phys., 5, 493–503, https://doi.org/10.5194/acp-5-493-2005, 2005.
Carrasco, N., Rayez, M. T., Rayez, J. C., and Doussin, J. F.: Experimental
and theoretical study of the reaction of OH radical with sabinene, Phys.
Chem. Chem. Phys., 8, 3211, https://doi.org/10.1039/b604489a, 2006.
Carrasco, N., Picquet-Varrault, B., and Doussin, J.-F.: Kinetic and product
study of the gas-phase reaction of sabinaketone with OH radical, Int. J.
Chem. Kinet., 39, 415–421, https://doi.org/10.1002/kin.20252, 2007.
Chiappini, L., Carrasco, N., Temine, B., Picquet-Varrault, B.,
Durand-Jolibois, R., Wenger, J. C., and Doussin, J.-F.: Gaseous and
Particulate Products from the Atmospheric Ozonolysis of a Biogenic
Hydrocarbon, Sabinene, Environ. Chem., 3, 286,
https://doi.org/10.1071/EN06037, 2006.
Cox, R. A., Ammann, M., Crowley, J. N., Herrmann, H., Jenkin, M. E., McNeill, V. F., Mellouki, A., Troe, J., and Wallington, T. J.: Evaluated kinetic and photochemical data for atmospheric chemistry: Volume VII – Criegee intermediates, Atmos. Chem. Phys., 20, 13497–13519, https://doi.org/10.5194/acp-20-13497-2020, 2020.
Crounse, J. D., Paulot, F., Kjaergaard, H. G., and Wennberg, P. O.: Peroxy
radical isomerization in the oxidation of isoprene, Phys. Chem. Chem. Phys.,
13, 13607–13613, https://doi.org/10.1039/C1CP21330J, 2011.
Crounse, J. D., Knap, H. C., Ørnsø, K. B., Jørgensen, S., Paulot,
F., Kjaergaard, H. G., and Wennberg, P. O.: Atmospheric Fate of
Methacrolein. 1. Peroxy Radical Isomerization Following Addition of OH and
O2, J. Phys. Chem. A, 116, 5756–5762, https://doi.org/10.1021/jp211560u,
2012.
da Silva, G., Graham, C., and Wang, Z.-F.: Unimolecular â-Hydroxyperoxy
Radical Decomposition with OH Recycling in the Photochemical Oxidation of
Isoprene, Environ. Sci. Technol., 44, 250–256,
https://doi.org/10.1021/es900924d, 2010.
Dorn, H.-P., Neuroth, R., and Hofzumahaus, A.: Investigation of OH
absorption cross sections of rotational transitions in the A2Σ,
Fuchs, H., Bohn, B., Hofzumahaus, A., Holland, F., Lu, K. D., Nehr, S., Rohrer, F., and Wahner, A.: Detection of HO2 by laser-induced fluorescence: calibration and interferences from RO2 radicals, Atmos. Meas. Tech., 4, 1209–1225, https://doi.org/10.5194/amt-4-1209-2011, 2011.
Fuchs, H., Hofzumahaus, A., Rohrer, F., Bohn, B., Brauers, T., Dorn, H.-P.,
Häseler, R., Holland, F., Kaminski, M., Li, X., Lu, K., Nehr, S.,
Tillmann, R., Wegener, R., and Wahner, A.: Experimental evidence for
efficient hydroxyl radical regeneration in isoprene oxidation, Nat. Geosci.,
6, 1023–1026, https://doi.org/10.1038/ngeo1964, 2013.
Fuchs, H., Acir, I.-H., Bohn, B., Brauers, T., Dorn, H.-P., Häseler, R.,
Hofzumahaus, A., Holland, F., Kaminski, M., Li, X., Lu, K., Lutz, A., Nehr,
S., Rohrer, F., Tillmann, R., Wegener, R., and Wahner, A.: OH regeneration
from methacrolein oxidation investigated in the atmosphere simulation
chamber SAPHIR, Atmos. Chem. Phys., 14, 7895–7908,
https://doi.org/10.5194/acp-14-7895-2014, 2014.
Fuchs, H., Novelli, A., Rolletter, M., Hofzumahaus, A., Pfannerstill, E. Y., Kessel, S., Edtbauer, A., Williams, J., Michoud, V., Dusanter, S., Locoge, N., Zannoni, N., Gros, V., Truong, F., Sarda-Esteve, R., Cryer, D. R., Brumby, C. A., Whalley, L. K., Stone, D., Seakins, P. W., Heard, D. E., Schoemaecker, C., Blocquet, M., Coudert, S., Batut, S., Fittschen, C., Thames, A. B., Brune, W. H., Ernest, C., Harder, H., Muller, J. B. A., Elste, T., Kubistin, D., Andres, S., Bohn, B., Hohaus, T., Holland, F., Li, X., Rohrer, F., Kiendler-Scharr, A., Tillmann, R., Wegener, R., Yu, Z., Zou, Q., and Wahner, A.: Comparison of OH reactivity measurements in the atmospheric simulation chamber SAPHIR, Atmos. Meas. Tech., 10, 4023–4053, https://doi.org/10.5194/amt-10-4023-2017, 2017.
Glowania, M., Rohrer, F., Dorn, H.-P., Hofzumahaus, A., Holland, F., Kiendler-Scharr, A., Wahner, A., and Fuchs, H.: Comparison of formaldehyde measurements by Hantzsch, CRDS and DOAS in the SAPHIR chamber, Atmos. Meas. Tech., 14, 4239–4253, https://doi.org/10.5194/amt-14-4239-2021, 2021.
Griffin, R. J., Cocker, D. R., Flagan, R. C., and Seinfeld, J. H.: Organic
aerosol formation from the oxidation of biogenic hydrocarbons, J. Geophys.
Res., 104, 3555–3567, https://doi.org/10.1029/1998JD100049, 1999.
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.
Hakola, H., Arey, J., Aschmann, S. M., and Atkinson, R.: Product formation
from the gas-phase reactions of OH radicals and O3 with a series of
monoterpenes, J. Atmos. Chem., 18, 75–102,
https://doi.org/10.1007/BF00694375, 1994.
Hakola, H., Rinne, J., and Laurila, T.: The hydrocarbon emission rates of
tea-leafed willow (Salix phylicifolia), silver birch (Betula pendula) and
European aspen (Populus tremula), Atmos. Environ., 32, 1825–1833,
https://doi.org/10.1016/S1352-2310(97)00482-2, 1998.
Hakola, H., Tarvainen, V., Laurila, T., Hiltunen, V., Hellén, H., and
Keronen, P.: Seasonal variation of VOC concentrations above a boreal
coniferous forest, Atmos. Environ., 37, 1623–1634,
https://doi.org/10.1016/S1352-2310(03)00014-1, 2003.
Hantschke, L., Novelli, A., Bohn, B., Cho, C., Reimer, D., Rohrer, F., Tillmann, R., Glowania, M., Hofzumahaus, A., Kiendler-Scharr, A., Wahner, A., and Fuchs, H.: Atmospheric photooxidation and ozonolysis of Δ3-carene and 3-caronaldehyde: rate constants and product yields, Atmos. Chem. Phys., 21, 12665–12685, https://doi.org/10.5194/acp-21-12665-2021, 2021.
Hofzumahaus, A., Rohrer, F., Lu, K., Bohn, B., Brauers, T., Chang, C.-C.,
Fuchs, H., Holland, F., Kita, K., Kondo, Y., Li, X., Lou, S., Shao, M.,
Zeng, L., Wahner, A., and Zhang, Y.: Amplified Trace Gas Removal in the
Troposphere, Science, 324, 1702–1704,
https://doi.org/10.1126/science.1164566, 2009.
Holzke, C., Dindorf, T., Kesselmeier, J., Kuhn, U., and Koppmann, R.:
Terpene emissions from European beech (shape Fagus sylvatica∼ L.): Pattern and Emission Behaviour Over two Vegetation Periods, J. Atmos.
Chem., 55, 81–102, https://doi.org/10.1007/s10874-006-9027-9, 2006.
Jenkin, M. E., Valorso, R., Aumont, B., Rickard, A. R., and Wallington, T. J.: Estimation of rate coefficients and branching ratios for gas-phase reactions of OH with aliphatic organic compounds for use in automated mechanism construction, Atmos. Chem. Phys., 18, 9297–9328, https://doi.org/10.5194/acp-18-9297-2018, 2018.
Jenkin, M. E., Valorso, R., Aumont, B., Newland, M. J., and Rickard, A. R.: Estimation of rate coefficients for the reactions of O3 with unsaturated organic compounds for use in automated mechanism construction, Atmos. Chem. Phys., 20, 12921–12937, https://doi.org/10.5194/acp-20-12921-2020, 2020.
Kaminski, M., Fuchs, H., Acir, I.-H., Bohn, B., Brauers, T., Dorn, H.-P., Häseler, R., Hofzumahaus, A., Li, X., Lutz, A., Nehr, S., Rohrer, F., Tillmann, R., Vereecken, L., Wegener, R., and Wahner, A.: Investigation of the β-pinene photooxidation by OH in the atmosphere simulation chamber SAPHIR, Atmos. Chem. Phys., 17, 6631–6650, https://doi.org/10.5194/acp-17-6631-2017, 2017.
Kim, J.-C., Kim, K.-J., Kim, D.-S., and Han, J.-S.: Seasonal variations of
monoterpene emissions from coniferous trees of different ages in Korea,
Chemosphere, 59, 1685–1696,
https://doi.org/10.1016/j.chemosphere.2004.10.048, 2005.
Kuwata, K. T., Luu, L., Weberg, A. B., Huang, K., Parsons, A. J., Peebles,
L. A., Rackstraw, N. B., and Kim, M. J.: Quantum Chemical and Statistical
Rate Theory Studies of the Vinyl Hydroperoxides Formed in trans-2-Butene
and 2,3-Dimethyl-2-butene Ozonolysis, J. Phys. Chem. A, 122, 2485–2502,
https://doi.org/10.1021/acs.jpca.8b00287, 2018.
Larsen, Bo. R., Di Bella, D., Glasius, M., Winterhalter, R., Jensen, N. R.,
and Hjorth, J.: Gas-Phase OH Oxidation of Monoterpenes: Gaseous and
Particulate Products, J. Atmos. Chem., 38, 231–276,
https://doi.org/10.1023/A:1006487530903, 2001.
Lee, A., Goldstein, A. H., Kroll, J. H., Ng, N. L., Varutbangkul, V.,
Flagan, R. C., and Seinfeld, J. H.: Gas-phase products and secondary aerosol
yields from the photooxidation of 16 different terpenes, J. Geophys. Res.,
111, D17305, https://doi.org/10.1029/2006JD007050, 2006.
Lelieveld, J., Butler, T. M., Crowley, J. N., Dillon, T. J., Fischer, H.,
Ganzeveld, L., Harder, H., Lawrence, M. G., Martinez, M., Taraborrelli, D.,
and Williams, J.: Atmospheric oxidation capacity sustained by a tropical
forest, Nature, 452, 737–740, https://doi.org/10.1038/nature06870, 2008.
Long, B., Bao, J. L., and Truhlar, D. G.: Atmospheric Chemistry of Criegee
Intermediates: Unimolecular Reactions and Reactions with Water, J. Am. Chem.
Soc., 138, 14409–14422, https://doi.org/10.1021/jacs.6b08655, 2016.
Lou, S., Holland, F., Rohrer, F., Lu, K., Bohn, B., Brauers, T., Chang, C. C., Fuchs, H., Häseler, R., Kita, K., Kondo, Y., Li, X., Shao, M., Zeng, L., Wahner, A., Zhang, Y., Wang, W., and Hofzumahaus, A.: Atmospheric OH reactivities in the Pearl River Delta – China in summer 2006: measurement and model results, Atmos. Chem. Phys., 10, 11243–11260, https://doi.org/10.5194/acp-10-11243-2010, 2010.
Ma, Y. and Marston, G.: Multifunctional acid formation from the gas-phase
ozonolysis of â-pinene, Phys. Chem. Chem. Phys., 10, 6115,
https://doi.org/10.1039/b807863g, 2008.
Mellouki, A., Ammann, M., Cox, R. A., Crowley, J. N., Herrmann, H., Jenkin, M. E., McNeill, V. F., Troe, J., and Wallington, T. J.: Evaluated kinetic and photochemical data for atmospheric chemistry: volume VIII – gas-phase reactions of organic species with four, or more, carbon atoms (≥C4), Atmos. Chem. Phys., 21, 4797–4808, https://doi.org/10.5194/acp-21-4797-2021, 2021.
Nguyen, T. B., Tyndall, G. S., Crounse, J. D., Teng, A. P., Bates, K. H.,
Schwantes, R. H., Coggon, M. M., Zhang, L., Feiner, P., Milller, D. O.,
Skog, K. M., Rivera-Rios, J. C., Dorris, M., Olson, K. F., Koss, A., Wild,
R. J., Brown, S. S., Goldstein, A. H., de Gouw, J. A., Brune, W. H.,
Keutsch, F. N., Seinfeld, J. H., and Wennberg, P. O.: Atmospheric fates of
Criegee intermediates in the ozonolysis of isoprene, Phys. Chem. Chem.
Phys., 18, 10241–10254, https://doi.org/10.1039/C6CP00053C, 2016.
Nguyen, T. L., Peeters, J., and Vereecken, L.: Theoretical study of the
gas-phase ozonolysis of β-pinene (C10H16), Phys. Chem. Chem. Phys., 11,
5643, https://doi.org/10.1039/b822984h, 2009.
Novelli, A., Vereecken, L., Bohn, B., Dorn, H.-P., Gkatzelis, G. I., Hofzumahaus, A., Holland, F., Reimer, D., Rohrer, F., Rosanka, S., Taraborrelli, D., Tillmann, R., Wegener, R., Yu, Z., Kiendler-Scharr, A., Wahner, A., and Fuchs, H.: Importance of isomerization reactions for OH radical regeneration from the photo-oxidation of isoprene investigated in the atmospheric simulation chamber SAPHIR, Atmos. Chem. Phys., 20, 3333–3355, https://doi.org/10.5194/acp-20-3333-2020, 2020.
Novelli, A., Pang, J. Y. S., Färber, M., Carlsson, P. T. M., Bohn, B.,
Gkatzelis, G. I., Rohrer, F., Wedel, S., and Fuchs, H.: Atmospheric simulation chamber study: Sabinene + O3 – Gas-phase oxidation – kinetic study (1.0) [data set], https://doi.org/10.25326/W4QV-KY95, 2023a.
Novelli, A., Pang, J. Y. S., Färber, M., Carlsson, P. T. M., Bohn, B.,
Gkatzelis, G. I., Rohrer, F., Wedel, S., and Fuchs, H.: Atmospheric
simulation chamber study: Sabinene + O3 – Gas-phase oxidation – kinetic
study (1.0) [data set], https://doi.org/10.25326/8BA6-MM58, 2023b.
Novelli, A., Pang, J. Y. S., Färber, M., Carlsson, P. T. M., Bohn, B.,
Gkatzelis, G. I., Rohrer, F., Wedel, S., and Fuchs, H.: Atmospheric
simulation chamber study: Sabinene + OH – Gas-phase oxidation – kinetic
study (1.0) [data set], https://doi.org/10.25326/QDQE-8Q79, 2023c.
Novelli, A., Pang, J. Y. S., Färber, M., Carlsson, P. T. M., Bohn, B.,
Gkatzelis, G. I., Rohrer, F., Wedel, S., and Fuchs, H.: Atmospheric
simulation chamber study: Sabinene + OH – Gas-phase oxidation – kinetic
study (1.0) [data set], https://doi.org/10.25326/25V8-PA77, 2023d.
Novelli, A., Pang, J. Y. S., Färber, M., Carlsson, P. T. M., Bohn, B.,
Gkatzelis, G. I., Rohrer, F., Wedel, S., and Fuchs, H.: Atmospheric
simulation chamber study: Sabinene + OH – Gas-phase oxidation – kinetic
study (1.0) [data set], https://doi.org/10.25326/FCYS-Y288, 2023e.
Novelli, A., Pang, J. Y. S., Färber, M., Carlsson, P. T. M., Bohn, B.,
Gkatzelis, G. I., Rohrer, F., Wedel, S., and Fuchs, H.: Atmospheric
simulation chamber study: Sabinene + OH – Gas-phase oxidation – kinetic
study (1.0) [data set], https://doi.org/10.25326/B5VV-K378, 2023f.
Novelli, A., Pang, J. Y. S., Färber, M., Carlsson, P. T. M., Bohn, B.,
Gkatzelis, G. I., Rohrer, F., Wedel, S., and Fuchs, H.: Atmospheric
simulation chamber study: Sabinene + OH – Gas-phase oxidation – kinetic
study (1.0) [data set], https://doi.org/10.25326/BQVM-QR53, 2023g.
Pang, J. Y. S., Novelli, A., Kaminski, M., Acir, I.-H., Bohn, B., Carlsson,
P. T. M., Cho, C., Dorn, H.-P., Hofzumahaus, A., Li, X., Lutz, A., Nehr, S.,
Reimer, D., Rohrer, F., Tillmann, R., Wegener, R., Kiendler-Scharr, A.,
Wahner, A., and Fuchs, H.: Investigation of the limonene photooxidation by
OH at different NO concentrations in the atmospheric simulation chamber
SAPHIR (Simulation of Atmospheric PHotochemistry In a large Reaction
Chamber), Atmos. Chem. Phys., 22, 8497–8527,
https://doi.org/10.5194/acp-22-8497-2022, 2022.
Peeters, J., Boullart, W., Pultau, V., Vandenberk, S., and Vereecken, L.:
Structure-Activity Relationship for the Addition of OH to (Poly)alkenes:
Site-Specific and Total Rate Constants, J. Phys. Chem. A, 111, 1618–1631,
https://doi.org/10.1021/jp066973o, 2007.
Peeters, J., Müller, J.-F., Stavrakou, T., and Nguyen, V. S.: Hydroxyl
Radical Recycling in Isoprene Oxidation Driven by Hydrogen Bonding and
Hydrogen Tunneling: The Upgraded LIM1 Mechanism, J. Phys. Chem. A, 118,
8625–8643, https://doi.org/10.1021/jp5033146, 2014.
Pfeifle, M., Ma, Y.-T., Jasper, A. W., Harding, L. B., Hase, W. L., and
Klippenstein, S. J.: Nascent energy distribution of the Criegee intermediate
CH2OO from direct dynamics calculations of primary ozonide dissociation, The
Journal of Chemical Physics, 148, 174306, https://doi.org/10.1063/1.5028117,
2018.
Reissell, A., Harry, C., Aschmann, S. M., Atkinson, R., and Arey, J.:
Formation of acetone from the OH radical- and O3-initiated reactions of a
series of monoterpenes, J. Geophys. Res., 104, 13869–13879,
https://doi.org/10.1029/1999JD900198, 1999.
Rohrer, F., Bohn, B., Brauers, T., Brüning, D., Johnen, F.-J., Wahner, A., and Kleffmann, J.: Characterisation of the photolytic HONO-source in the atmosphere simulation chamber SAPHIR, Atmos. Chem. Phys., 5, 2189–2201, https://doi.org/10.5194/acp-5-2189-2005, 2005.
Rolletter, M., Kaminski, M., Acir, I.-H., Bohn, B., Dorn, H.-P., Li, X., Lutz, A., Nehr, S., Rohrer, F., Tillmann, R., Wegener, R., Hofzumahaus, A., Kiendler-Scharr, A., Wahner, A., and Fuchs, H.: Investigation of the α-pinene photooxidation by OH in the atmospheric simulation chamber SAPHIR, Atmos. Chem. Phys., 19, 11635–11649, https://doi.org/10.5194/acp-19-11635-2019, 2019.
Rollins, A. W., Smith, J. D., Wilson, K. R., and Cohen, R. C.: Real Time In
Situ Detection of Organic Nitrates in Atmospheric Aerosols, Environ. Sci.
Technol., 44, 5540–5545, https://doi.org/10.1021/es100926x, 2010.
Sekimoto, K., Li, S.-M., Yuan, B., Koss, A., Coggon, M., Warneke, C., and De
Gouw, J.: Calculation of the sensitivity of proton-transfer-reaction mass
spectrometry (PTR-MS) for organic trace gases using molecular properties,
Int. J. Mass Spectrom., 421, 71–94,
https://doi.org/10.1016/j.ijms.2017.04.006, 2017.
Sindelarova, K., Granier, C., Bouarar, I., Guenther, A., Tilmes, S., Stavrakou, T., Müller, J.-F., Kuhn, U., Stefani, P., and Knorr, W.: Global data set of biogenic VOC emissions calculated by the MEGAN model over the last 30 years, Atmos. Chem. Phys., 14, 9317–9341, https://doi.org/10.5194/acp-14-9317-2014, 2014.
Staudt, M. and Bertin, N.: Light and temperature dependence of the emission
of cyclic and acyclic monoterpenes from holm oak (Quercus ilex L.) leaves,
Plant Cell Environ., 21, 385–395,
https://doi.org/10.1046/j.1365-3040.1998.00288.x, 1998.
Tollsten, L. and Müller, P. M.: Volatile organic compounds emitted from
beech leaves, Phytochem., 43, 759–762,
https://doi.org/10.1016/0031-9422(96)00272-5, 1996.
Vereecken, L. and Nozière, B.: H migration in peroxy radicals under atmospheric conditions, Atmos. Chem. Phys., 20, 7429–7458, https://doi.org/10.5194/acp-20-7429-2020, 2020.
Vereecken, L. and Peeters, J.: A theoretical study of the OH-initiated
gas-phase oxidation mechanism of β-pinene (C10H16): first generation
products, Phys. Chem. Chem. Phys., 14, 3802,
https://doi.org/10.1039/c2cp23711c, 2012.
Vereecken, L., Novelli, A., and Taraborrelli, D.: Unimolecular decay
strongly limits the atmospheric impact of Criegee intermediates, Phys. Chem.
Chem. Phys., 19, 31599–31612, https://doi.org/10.1039/C7CP05541B, 2017.
Wang, L. and Wang, L.: Mechanism of gas-phase ozonolysis of sabinene in the
atmosphere, Phys. Chem. Chem. Phys., 19, 24209–24218,
https://doi.org/10.1039/C7CP03216A, 2017.
Wang, L. and Wang, L.: Atmospheric Oxidation Mechanism of Sabinene Initiated
by the Hydroxyl Radicals, J. Phys. Chem. A, 122, 8783–8793,
https://doi.org/10.1021/acs.jpca.8b06381, 2018.
Whalley, L. K., Edwards, P. M., Furneaux, K. L., Goddard, A., Ingham, T., Evans, M. J., Stone, D., Hopkins, J. R., Jones, C. E., Karunaharan, A., Lee, J. D., Lewis, A. C., Monks, P. S., Moller, S. J., and Heard, D. E.: Quantifying the magnitude of a missing hydroxyl radical source in a tropical rainforest, Atmos. Chem. Phys., 11, 7223–7233, https://doi.org/10.5194/acp-11-7223-2011, 2011.
Xu, L., Møller, K. H., Crounse, J. D., Otkjær, R. V., Kjaergaard, H.
G., and Wennberg, P. O.: Unimolecular Reactions of Peroxy Radicals Formed in
the Oxidation of β-Pinene and β-Pinene by Hydroxyl Radicals, J.
Phys. Chem. A, 123, 1661–1674, https://doi.org/10.1021/acs.jpca.8b11726,
2019.
Yu, J., Cocker III, D. R., Griffin, R. J., Flagan, R. C., and Seinfeld, J.
H.: Gas-Phase Ozone Oxidation of Monoterpenes: Gaseous and Particulate
Products, J. Atmos. Chem., 34, 207–258,
https://doi.org/10.1023/A:1006254930583, 1999.
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.
In this study, the oxidations of sabinene by OH radicals and ozone were investigated with an...
Altmetrics
Final-revised paper
Preprint