Articles | Volume 14, issue 6
https://doi.org/10.5194/amt-14-4239-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/amt-14-4239-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
09 Jun 2021
Research article |
| 09 Jun 2021
| 09 Jun 2021
Comparison of formaldehyde measurements by Hantzsch, CRDS and DOAS in the SAPHIR chamber
Marvin Glowania
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
Hans-Peter Dorn
Institute of Energy and Climate Research, IEK-8: Troposphere, Forschungszentrum Jülich GmbH, Jülich, Germany
Andreas Hofzumahaus
Institute of Energy and Climate Research, IEK-8: Troposphere, Forschungszentrum Jülich GmbH, Jülich, Germany
Frank Holland
Institute of Energy and Climate Research, IEK-8: Troposphere, Forschungszentrum Jülich GmbH, Jülich, Germany
Astrid Kiendler-Scharr
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
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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.
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EGUsphere, https://doi.org/10.5194/egusphere-2025-450, https://doi.org/10.5194/egusphere-2025-450, 2025
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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.
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
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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
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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.
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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
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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
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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.
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
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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.
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
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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
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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
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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
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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
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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
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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
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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
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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.
Andrea Pozzer, Simon F. Reifenberg, Vinod Kumar, Bruno Franco, Matthias Kohl, Domenico Taraborrelli, Sergey Gromov, Sebastian Ehrhart, Patrick Jöckel, Rolf Sander, Veronica Fall, Simon Rosanka, Vlassis Karydis, Dimitris Akritidis, Tamara Emmerichs, Monica Crippa, Diego Guizzardi, Johannes W. Kaiser, Lieven Clarisse, Astrid Kiendler-Scharr, Holger Tost, and Alexandra Tsimpidi
Geosci. Model Dev., 15, 2673–2710, https://doi.org/10.5194/gmd-15-2673-2022, https://doi.org/10.5194/gmd-15-2673-2022, 2022
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A newly developed setup of the chemistry general circulation model EMAC (ECHAM5/MESSy for Atmospheric Chemistry) is evaluated here. A comprehensive organic degradation mechanism is used and coupled with a volatility base model.
The results show that the model reproduces most of the tracers and aerosols satisfactorily but shows discrepancies for oxygenated organic gases. It is also shown that this model configuration can be used for further research in atmospheric chemistry.
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
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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.
Zhi-Hui Zhang, Elena Hartner, Battist Utinger, Benjamin Gfeller, Andreas Paul, Martin Sklorz, Hendryk Czech, Bin Xia Yang, Xin Yi Su, Gert Jakobi, Jürgen Orasche, Jürgen Schnelle-Kreis, Seongho Jeong, Thomas Gröger, Michal Pardo, Thorsten Hohaus, Thomas Adam, Astrid Kiendler-Scharr, Yinon Rudich, Ralf Zimmermann, and Markus Kalberer
Atmos. Chem. Phys., 22, 1793–1809, https://doi.org/10.5194/acp-22-1793-2022, https://doi.org/10.5194/acp-22-1793-2022, 2022
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Using a novel setup, we comprehensively characterized the formation of particle-bound reactive oxygen species (ROS) in anthropogenic and biogenic secondary organic aerosols (SOAs). We found that more than 90 % of all ROS components in both SOA types have a short lifetime. Our results also show that photochemical aging promotes particle-bound ROS production and enhances the oxidative potential of the aerosols. We found consistent results between chemical-based and biological-based ROS analyses.
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
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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
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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
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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
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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
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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
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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
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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
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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.
Clara Betancourt, Christoph Küppers, Tammarat Piansawan, Uta Sager, Andrea B. Hoyer, Heinz Kaminski, Gerhard Rapp, Astrid C. John, Miriam Küpper, Ulrich Quass, Thomas Kuhlbusch, Jochen Rudolph, Astrid Kiendler-Scharr, and Iulia Gensch
Atmos. Chem. Phys., 21, 5953–5964, https://doi.org/10.5194/acp-21-5953-2021, https://doi.org/10.5194/acp-21-5953-2021, 2021
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For the first time, we included stable isotopes in the Lagrangian particle dispersion model FLEXPART to investigate firewood home heating aerosol. This is an innovative source apportionment methodology since comparison of stable isotope ratio model predictions with observations delivers quantitative understanding of atmospheric processes. The main outcome of this study is that the home heating aerosol in residential areas was not of remote origin.
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
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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.
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
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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
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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.
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
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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
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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.
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
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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
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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.
Andreas Petzold, Patrick Neis, Mihal Rütimann, Susanne Rohs, Florian Berkes, Herman G. J. Smit, Martina Krämer, Nicole Spelten, Peter Spichtinger, Philippe Nédélec, and Andreas Wahner
Atmos. Chem. Phys., 20, 8157–8179, https://doi.org/10.5194/acp-20-8157-2020, https://doi.org/10.5194/acp-20-8157-2020, 2020
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The first analysis of 15 years of global-scale water vapour and relative humidity observations by passenger aircraft in the MOZAIC and IAGOS programmes resolves detailed features of water vapour and ice-supersaturated air in the mid-latitude tropopause. Key results provide in-depth insight into seasonal and regional variability and chemical signatures of ice-supersaturated air masses, including trend analyses, and show a close link to cirrus clouds and their highly important effects on climate.
Anna Novelli, Luc Vereecken, Birger Bohn, Hans-Peter Dorn, Georgios I. Gkatzelis, Andreas Hofzumahaus, Frank Holland, David Reimer, Franz Rohrer, Simon Rosanka, Domenico Taraborrelli, Ralf Tillmann, Robert Wegener, Zhujun Yu, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 20, 3333–3355, https://doi.org/10.5194/acp-20-3333-2020, https://doi.org/10.5194/acp-20-3333-2020, 2020
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Experimental evidence from a simulation chamber study shows that the regeneration efficiency of the hydroxyl radical is maintained globally at values higher than 0.5 for a wide range of nitrogen oxide concentrations as a result of isomerizations of peroxy radicals originating from the OH oxidation of isoprene. The available models were tested, and suggestions on how to improve their ability to reproduce the measured radical and oxygenated volatile organic compound concentrations are provided.
Yu Wang, Ying Chen, Zhijun Wu, Dongjie Shang, Yuxuan Bian, Zhuofei Du, Sebastian H. Schmitt, Rong Su, Georgios I. Gkatzelis, Patrick Schlag, Thorsten Hohaus, Aristeidis Voliotis, Keding Lu, Limin Zeng, Chunsheng Zhao, M. Rami Alfarra, Gordon McFiggans, Alfred Wiedensohler, Astrid Kiendler-Scharr, Yuanhang Zhang, and Min Hu
Atmos. Chem. Phys., 20, 2161–2175, https://doi.org/10.5194/acp-20-2161-2020, https://doi.org/10.5194/acp-20-2161-2020, 2020
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Severe haze events, with high particulate nitrate (pNO3−) burden, frequently prevail in Beijing. In this study, we demonstrate a mutual-promotion effect between aerosol water uptake and pNO3− formation backed up by theoretical calculations and field observations throughout a typical pNO3−-dominated haze event in Beijing wintertime. This self-amplified mutual-promotion effect between aerosol water content and particulate nitrate can rapidly deteriorate air quality and degrade visibility.
Olga Garmash, Matti P. Rissanen, Iida Pullinen, Sebastian Schmitt, Oskari Kausiala, Ralf Tillmann, Defeng Zhao, Carl Percival, Thomas J. Bannan, Michael Priestley, Åsa M. Hallquist, Einhard Kleist, Astrid Kiendler-Scharr, Mattias Hallquist, Torsten Berndt, Gordon McFiggans, Jürgen Wildt, Thomas F. Mentel, and Mikael Ehn
Atmos. Chem. Phys., 20, 515–537, https://doi.org/10.5194/acp-20-515-2020, https://doi.org/10.5194/acp-20-515-2020, 2020
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Highly oxygenated organic molecules (HOMs) facilitate aerosol formation in the atmosphere. Using NO3− chemical ionization mass spectrometry we investigated HOM composition and yield in oxidation of aromatic compounds at different reactant concentrations, in the presence of NOx and seed aerosol. Higher OH concentrations increased HOM yield, suggesting multiple oxidation steps, and affected HOM composition, potentially explaining in part discrepancies in published secondary organic aerosol yields.
Rupert Holzinger, W. Joe F. Acton, William J. Bloss, Martin Breitenlechner, Leigh R. Crilley, Sébastien Dusanter, Marc Gonin, Valerie Gros, Frank N. Keutsch, Astrid Kiendler-Scharr, Louisa J. Kramer, Jordan E. Krechmer, Baptiste Languille, Nadine Locoge, Felipe Lopez-Hilfiker, Dušan Materić, Sergi Moreno, Eiko Nemitz, Lauriane L. J. Quéléver, Roland Sarda Esteve, Stéphane Sauvage, Simon Schallhart, Roberto Sommariva, Ralf Tillmann, Sergej Wedel, David R. Worton, Kangming Xu, and Alexander Zaytsev
Atmos. Meas. Tech., 12, 6193–6208, https://doi.org/10.5194/amt-12-6193-2019, https://doi.org/10.5194/amt-12-6193-2019, 2019
Michael Rolletter, Martin Kaminski, Ismail-Hakki Acir, Birger Bohn, Hans-Peter Dorn, Xin Li, Anna Lutz, Sascha Nehr, Franz Rohrer, Ralf Tillmann, Robert Wegener, Andreas Hofzumahaus, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 19, 11635–11649, https://doi.org/10.5194/acp-19-11635-2019, https://doi.org/10.5194/acp-19-11635-2019, 2019
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Here we present a study of the photooxidation of alpha-pinene, the most abundant monoterpene, by hydroxyl radicals (OH) conducted in the simulation chamber SAPHIR under low NOx and atmospheric alpha-pinene concentrations. Yields of the main degradation products acetone, formaldehyde, and pinonaldehyde were determined and the HOx (OH + HO2) radical budget was investigated. Measurements were used to test current atmospheric models and a theory-based mechanism.
Zhaofeng Tan, Keding Lu, Andreas Hofzumahaus, Hendrik Fuchs, Birger Bohn, Frank Holland, Yuhan Liu, Franz Rohrer, Min Shao, Kang Sun, Yusheng Wu, Limin Zeng, Yinsong Zhang, Qi Zou, Astrid Kiendler-Scharr, Andreas Wahner, and Yuanhang Zhang
Atmos. Chem. Phys., 19, 7129–7150, https://doi.org/10.5194/acp-19-7129-2019, https://doi.org/10.5194/acp-19-7129-2019, 2019
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Atmospheric OH, HO2, and RO2 radicals; OH reactivity; and trace gases measured in the Pearl River Delta in autumn 2014 are used for radical budget analyses. The RO2 budget suggests that unexplained OH reactivity is due to unmeasured volatile organic compounds. The OH budget points to a missing OH source and that of RO2 to a missing RO2 sink at low NO. This could indicate a common, unknown process that converts RO2 to OH without the involvement of NO, which would reduce ozone production by 30 %.
Ralph Dlugi, Martina Berger, Chinmay Mallik, Anywhere Tsokankunku, Michael Zelger, Otávio C. Acevedo, Efstratios Bourtsoukidis, Andreas Hofzumahaus, Jürgen Kesselmeier, Gerhard Kramm, Daniel Marno, Monica Martinez, Anke C. Nölscher, Huug Ouwersloot, Eva Y. Pfannerstill, Franz Rohrer, Sebastian Tauer, Jonathan Williams, Ana-Maria Yáñez-Serrano, Meinrat O. Andreae, Hartwig Harder, and Matthias Sörgel
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-1325, https://doi.org/10.5194/acp-2018-1325, 2019
Publication in ACP not foreseen
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Incomplete mixing (segregation) results in reduced chemical reaction rates compared to those expected from mean values and rate constants. Segregation has been suggested to cause discrepancies between modelled and measured OH radical concentrations. In this work, we summarize the intensities of segregation for the reaction of OH and isoprene for different field and modelling studies and compare those to our results from measurements in a pristine environment.
Sascha R. Albrecht, Anna Novelli, Andreas Hofzumahaus, Sungah Kang, Yare Baker, Thomas Mentel, Andreas Wahner, and Hendrik Fuchs
Atmos. Meas. Tech., 12, 891–902, https://doi.org/10.5194/amt-12-891-2019, https://doi.org/10.5194/amt-12-891-2019, 2019
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Within this study we demonstrate reliable measurement of hydroperoxy (HO2) radicals via chemical ionisation mass spectrometry. HO2 is detected as an ion cluster with bromide ions, which allows a selective detection. This direct and sensitive measurement provides reliable data of HO2 radical concentrations in the atmosphere as demonstrated in the first application in simulation chamber experiments.
Georgios I. Gkatzelis, Thorsten Hohaus, Ralf Tillmann, Iulia Gensch, Markus Müller, Philipp Eichler, Kang-Ming Xu, Patrick Schlag, Sebastian H. Schmitt, Zhujun Yu, Robert Wegener, Martin Kaminski, Rupert Holzinger, Armin Wisthaler, and Astrid Kiendler-Scharr
Atmos. Chem. Phys., 18, 12969–12989, https://doi.org/10.5194/acp-18-12969-2018, https://doi.org/10.5194/acp-18-12969-2018, 2018
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Defining the fundamental parameters that distribute organic molecules between the gas and particle phases is essential to understand their impact on the atmosphere. In this work, gas to particle partitioning of major biogenic oxidation products from monoterpenes and real plant emissions was investigated. While measurement results and theoretical calculation for most semi-volatile compounds are in good agreement, significant deviations are found for intermediate volatile organic compounds.
Zhaofeng Tan, Franz Rohrer, Keding Lu, Xuefei Ma, Birger Bohn, Sebastian Broch, Huabin Dong, Hendrik Fuchs, Georgios I. Gkatzelis, Andreas Hofzumahaus, Frank Holland, Xin Li, Ying Liu, Yuhan Liu, Anna Novelli, Min Shao, Haichao Wang, Yusheng Wu, Limin Zeng, Min Hu, Astrid Kiendler-Scharr, Andreas Wahner, and Yuanhang Zhang
Atmos. Chem. Phys., 18, 12391–12411, https://doi.org/10.5194/acp-18-12391-2018, https://doi.org/10.5194/acp-18-12391-2018, 2018
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We present the first wintertime OH, HO2, and RO2 measurements in Beijing, China. OH concentrations are nearly 2-fold larger than those observed in foreign cities during wintertime. The high OH and large OH reactivities indicate photochemical processes can be effective even during wintertime. A box model largely underestimated HO2 and RO2 concentrations during pollution episodes correlated with high NOx, indicating a deficit current chemistry in the high NOx regime.
Hongyu Guo, Rene Otjes, Patrick Schlag, Astrid Kiendler-Scharr, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 18, 12241–12256, https://doi.org/10.5194/acp-18-12241-2018, https://doi.org/10.5194/acp-18-12241-2018, 2018
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Reduction in ammonia has been proposed as a way to lower fine particle mass and improve air quality, but gas-phase ammonia is linked to agricultural productivity. We assess the feasibility of ammonia control at a variety of locations through an aerosol thermodynamic analysis. We show that aerosol response to ammonia control is highly nonlinear and only becomes effective when ambient particle pH drops below approximately 3. Particle pH is a relevant aerosol air quality parameter.
Anna Novelli, Martin Kaminski, Michael Rolletter, Ismail-Hakki Acir, Birger Bohn, Hans-Peter Dorn, Xin Li, Anna Lutz, Sascha Nehr, Franz Rohrer, Ralf Tillmann, Robert Wegener, Frank Holland, Andreas Hofzumahaus, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 18, 11409–11422, https://doi.org/10.5194/acp-18-11409-2018, https://doi.org/10.5194/acp-18-11409-2018, 2018
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The impact of photooxidation of 2-methyl-3-butene-2-ol (MBO) on the concentration of radical species was studied in the atmospheric simulation chamber SAPHIR. MBO is a volatile organic compound mainly emitted by ponderosa and lodgepole pines which are very abundant in forests in the central-west USA. A very good agreement between measured and modelled radical concentrations and products from the oxidation of MBO was observed in an environment with NO of ~ 200 pptv.
Eleni Karnezi, Benjamin N. Murphy, Laurent Poulain, Hartmut Herrmann, Alfred Wiedensohler, Florian Rubach, Astrid Kiendler-Scharr, Thomas F. Mentel, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 10759–10772, https://doi.org/10.5194/acp-18-10759-2018, https://doi.org/10.5194/acp-18-10759-2018, 2018
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Different parameterizations of the organic aerosol (OA) formation and evolution are evaluated using ground and airborne measurements collected in the 2012 PEGASOS field campaign in the Po Valley (Italy). Total OA concentration and O : C ratios were reproduced within experimental error by a number of schemes. Anthropogenic secondary OA (SOA) contributed 15–25 % of the total OA, 20–35 % of SOA from intermediate volatility compounds oxidation, and 15–45 % of biogenic SOA depending on the scheme.
Florian Berkes, Norbert Houben, Ulrich Bundke, Harald Franke, Hans-Werner Pätz, Franz Rohrer, Andreas Wahner, and Andreas Petzold
Atmos. Meas. Tech., 11, 3737–3757, https://doi.org/10.5194/amt-11-3737-2018, https://doi.org/10.5194/amt-11-3737-2018, 2018
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The need for in situ nitrogen oxide measurements on a global scale is crucial to improve the chemistry in global chemistry models and evaluate satellite retrievals. Here we present the characterization of the new IAGOS NOx instrument installed on passenger aircraft, which will provide statistical robust measurements from the surface up to 13 km.
Hendrik Fuchs, Sascha Albrecht, Ismail–Hakki Acir, Birger Bohn, Martin Breitenlechner, Hans-Peter Dorn, Georgios I. Gkatzelis, Andreas Hofzumahaus, Frank Holland, Martin Kaminski, Frank N. Keutsch, Anna Novelli, David Reimer, Franz Rohrer, Ralf Tillmann, Luc Vereecken, Robert Wegener, Alexander Zaytsev, Astrid Kiendler-Scharr, and Andreas Wahner
Atmos. Chem. Phys., 18, 8001–8016, https://doi.org/10.5194/acp-18-8001-2018, https://doi.org/10.5194/acp-18-8001-2018, 2018
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The photooxidation of methyl vinyl ketone MVK, one of the most important products of isoprene that is emitted by plants, was investigated in the atmospheric simulation chamber SAPHIR for conditions found in forested areas. The comparison of measured trace gas time series with model calculations shows a gap in the understanding of radical chemistry in the MVK oxidation scheme. The possibility of unimolecular isomerization reactions were investigated by means of quantum-chemical calculations.
Mingjin Wang, Tong Zhu, Defeng Zhao, Florian Rubach, Andreas Wahner, Astrid Kiendler-Scharr, and Thomas F. Mentel
Atmos. Chem. Phys., 18, 7345–7359, https://doi.org/10.5194/acp-18-7345-2018, https://doi.org/10.5194/acp-18-7345-2018, 2018
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Organic coatings modify hygroscopicity and CCN activation of mineral dust perticles. Small amounts of oleic acid coating (volume fraction (vf) ≤ 4.1 %) decreased the CCN activity of CaCO3 particles, while more oleic acid coating (vf ≥ 14.8 %) increased the CCN activity of CaCO3 particles, while malonic acid coating (vf = 0.4−42 %) even in smallest amounts increased the CCN activity of CaCO3 particles. Our laboratory results should also hold under conditions of the atmosphere.
Georgios I. Gkatzelis, Ralf Tillmann, Thorsten Hohaus, Markus Müller, Philipp Eichler, Kang-Ming Xu, Patrick Schlag, Sebastian H. Schmitt, Robert Wegener, Martin Kaminski, Rupert Holzinger, Armin Wisthaler, and Astrid Kiendler-Scharr
Atmos. Meas. Tech., 11, 1481–1500, https://doi.org/10.5194/amt-11-1481-2018, https://doi.org/10.5194/amt-11-1481-2018, 2018
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This manuscript presents an intercomparison of state-of-the-art online and in situ particle sampling techniques connected to proton transfer reaction time-of-flight mass spectrometry (PTR-ToF-MS). Collection and vaporization of aerosol combined with soft ionization mass spectrometry offers the advantage of detailed chemical characterization of SOA species. The benefits of these techniques are highlighted through their consistency in providing the chemical composition of biogenic SOA.
Defeng Zhao, Sebastian H. Schmitt, Mingjin Wang, Ismail-Hakki Acir, Ralf Tillmann, Zhaofeng Tan, Anna Novelli, Hendrik Fuchs, Iida Pullinen, Robert Wegener, Franz Rohrer, Jürgen Wildt, Astrid Kiendler-Scharr, Andreas Wahner, and Thomas F. Mentel
Atmos. Chem. Phys., 18, 1611–1628, https://doi.org/10.5194/acp-18-1611-2018, https://doi.org/10.5194/acp-18-1611-2018, 2018
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Air pollutants emitted by human activities such as NOx and SO2 can influence the abundance of secondary organic aerosol (SOA) from biogenic volatile organic compounds (VOCs). We found that NOx suppressed new particle formation and SOA mass formation. When both SO2 and NOx are present, the suppressing effect of NOx on SOA mass formation was counteracted by SO2. High NOx changed SOA chemical composition, forming more organic nitrate, because NOx changed radical chemistry during VOC oxidation.
Hendrik Fuchs, Anna Novelli, Michael Rolletter, Andreas Hofzumahaus, Eva Y. Pfannerstill, Stephan Kessel, Achim Edtbauer, Jonathan Williams, Vincent Michoud, Sebastien Dusanter, Nadine Locoge, Nora Zannoni, Valerie Gros, Francois Truong, Roland Sarda-Esteve, Danny R. Cryer, Charlotte A. Brumby, Lisa K. Whalley, Daniel Stone, Paul W. Seakins, Dwayne E. Heard, Coralie Schoemaecker, Marion Blocquet, Sebastien Coudert, Sebastien Batut, Christa Fittschen, Alexander B. Thames, William H. Brune, Cheryl Ernest, Hartwig Harder, Jennifer B. A. Muller, Thomas Elste, Dagmar Kubistin, Stefanie Andres, Birger Bohn, Thorsten Hohaus, Frank Holland, Xin Li, Franz Rohrer, Astrid Kiendler-Scharr, Ralf Tillmann, Robert Wegener, Zhujun Yu, Qi Zou, and Andreas Wahner
Atmos. Meas. Tech., 10, 4023–4053, https://doi.org/10.5194/amt-10-4023-2017, https://doi.org/10.5194/amt-10-4023-2017, 2017
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Hydroxyl radical reactivity (k(OH)) is closely related to processes that lead to the formation of oxidised, secondary pollutants such as ozone and aerosol. In order to compare the performances of instruments measuring k(OH), experiments were conducted in the simulation chamber SAPHIR. Chemical conditions were chosen either to be representative of the atmosphere or to test potential limitations of instruments. Overall, the results show that instruments are capable of measuring k(OH).
Florian Berkes, Patrick Neis, Martin G. Schultz, Ulrich Bundke, Susanne Rohs, Herman G. J. Smit, Andreas Wahner, Paul Konopka, Damien Boulanger, Philippe Nédélec, Valerie Thouret, and Andreas Petzold
Atmos. Chem. Phys., 17, 12495–12508, https://doi.org/10.5194/acp-17-12495-2017, https://doi.org/10.5194/acp-17-12495-2017, 2017
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This study highlights the importance of independent global measurements with high and long-term accuracy to quantify long-term changes, especially in the UTLS region, and to help identify inconsistencies between different data sets of observations and models. Here we investigated temperature trends over different regions within a climate-sensitive area of the atmosphere and demonstrated the value of the IAGOS temperature observations as an anchor point for the evaluation of reanalyses.
Cheng Wu, Iida Pullinen, Stefanie Andres, Astrid Kiendler-Scharr, Einhard Kleist, Andreas Wahner, Jürgen Wildt, and Thomas F. Mentel
Biogeosciences Discuss., https://doi.org/10.5194/bg-2017-260, https://doi.org/10.5194/bg-2017-260, 2017
Manuscript not accepted for further review
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Biogenic volatile organic compounds are important for atmospheric chemistry. We showed by 13CO2 labelling experiments that biosynthesis is not restricted to the presence of light. In particular sesquiterpenes exhibit substantial de novo emissions in darkness with the carbon being delivered from alternative carbon sources. Our findings are of importance for future emissions under conditions of climate change as the response of de novo emissions to stresses differs from that of pool emissions.
Martin Kaminski, Hendrik Fuchs, Ismail-Hakki Acir, Birger Bohn, Theo Brauers, Hans-Peter Dorn, Rolf Häseler, Andreas Hofzumahaus, Xin Li, Anna Lutz, Sascha Nehr, Franz Rohrer, Ralf Tillmann, Luc Vereecken, Robert Wegener, and Andreas Wahner
Atmos. Chem. Phys., 17, 6631–6650, https://doi.org/10.5194/acp-17-6631-2017, https://doi.org/10.5194/acp-17-6631-2017, 2017
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Monoterpenes emitted by trees are among the volatile organic compounds with the highest global emission rates. The atmospheric degradation of the monoterpene β-pinene was investigated in the atmosphere simulation chamber SAPHIR in Jülich under low NOx and atmospheric β-pinene concentrations. While the budget of OH was balanced, both OH and HO2 concentrations were underestimated in the simulation results. These observations suggest the existence of unaccounted sources of HO2.
Nga Lee Ng, Steven S. Brown, Alexander T. Archibald, Elliot Atlas, Ronald C. Cohen, John N. Crowley, Douglas A. Day, Neil M. Donahue, Juliane L. Fry, Hendrik Fuchs, Robert J. Griffin, Marcelo I. Guzman, Hartmut Herrmann, Alma Hodzic, Yoshiteru Iinuma, José L. Jimenez, Astrid Kiendler-Scharr, Ben H. Lee, Deborah J. Luecken, Jingqiu Mao, Robert McLaren, Anke Mutzel, Hans D. Osthoff, Bin Ouyang, Benedicte Picquet-Varrault, Ulrich Platt, Havala O. T. Pye, Yinon Rudich, Rebecca H. Schwantes, Manabu Shiraiwa, Jochen Stutz, Joel A. Thornton, Andreas Tilgner, Brent J. Williams, and Rahul A. Zaveri
Atmos. Chem. Phys., 17, 2103–2162, https://doi.org/10.5194/acp-17-2103-2017, https://doi.org/10.5194/acp-17-2103-2017, 2017
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Oxidation of biogenic volatile organic compounds by NO3 is an important interaction between anthropogenic
and natural emissions. This review results from a June 2015 workshop and includes the recent literature
on kinetics, mechanisms, organic aerosol yields, and heterogeneous chemistry; advances in analytical
instrumentation; the current state NO3-BVOC chemistry in atmospheric models; and critical needs for
future research in modeling, field observations, and laboratory studies.
Zhaofeng Tan, Hendrik Fuchs, Keding Lu, Andreas Hofzumahaus, Birger Bohn, Sebastian Broch, Huabin Dong, Sebastian Gomm, Rolf Häseler, Lingyan He, Frank Holland, Xin Li, Ying Liu, Sihua Lu, Franz Rohrer, Min Shao, Baolin Wang, Ming Wang, Yusheng Wu, Limin Zeng, Yinsong Zhang, Andreas Wahner, and Yuanhang Zhang
Atmos. Chem. Phys., 17, 663–690, https://doi.org/10.5194/acp-17-663-2017, https://doi.org/10.5194/acp-17-663-2017, 2017
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In this study, we performed accurate OH measurements as well as selective HO2 and RO2 measurements at a rural site in North China Plain with state-of-the-art instruments newly developed. We confirmed the previous discovery on the enhancement of the OH in low NOx with which little O3 production was associated, and we found a missing RO2 source in high NOx which promoted higher O3 production. Our results are of vital importance for ozone abatement strategies currently under discussion for China.
Hendrik Fuchs, Zhaofeng Tan, Keding Lu, Birger Bohn, Sebastian Broch, Steven S. Brown, Huabin Dong, Sebastian Gomm, Rolf Häseler, Lingyan He, Andreas Hofzumahaus, Frank Holland, Xin Li, Ying Liu, Sihua Lu, Kyung-Eun Min, Franz Rohrer, Min Shao, Baolin Wang, Ming Wang, Yusheng Wu, Limin Zeng, Yinson Zhang, Andreas Wahner, and Yuanhang Zhang
Atmos. Chem. Phys., 17, 645–661, https://doi.org/10.5194/acp-17-645-2017, https://doi.org/10.5194/acp-17-645-2017, 2017
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OH reactivity was measured during a 1-month long campaign at a rural site in the North China Plain in 2014. OH reactivity measurements are compared to calculations using OH reactant measurements. Good agreement is found indicating that all important OH reactants were measured. In addition, the chemical OH budget is analyzed. In contrast to previous campaigns in China in 2006, no significant imbalance between OH production and destruction is found.
Weiwei Hu, Brett B. Palm, Douglas A. Day, Pedro Campuzano-Jost, Jordan E. Krechmer, Zhe Peng, Suzane S. de Sá, Scot T. Martin, M. Lizabeth Alexander, Karsten Baumann, Lina Hacker, Astrid Kiendler-Scharr, Abigail R. Koss, Joost A. de Gouw, Allen H. Goldstein, Roger Seco, Steven J. Sjostedt, Jeong-Hoo Park, Alex B. Guenther, Saewung Kim, Francesco Canonaco, André S. H. Prévôt, William H. Brune, and Jose L. Jimenez
Atmos. Chem. Phys., 16, 11563–11580, https://doi.org/10.5194/acp-16-11563-2016, https://doi.org/10.5194/acp-16-11563-2016, 2016
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IEPOX-SOA is biogenically derived secondary organic aerosol under anthropogenic influence, which has been shown to comprise a substantial fraction of OA globally. We investigated the lifetime of ambient IEPOX-SOA in the SE US and Amazonia, with an oxidation flow reactor and thermodenuder coupled with MS-based instrumentation. The low volatility and long lifetime of IEPOX-SOA against OH radicals' oxidation (> 2 weeks) was observed, which can help to constrain OA impact on air quality and climate.
Mehrnaz Sarrafzadeh, Jürgen Wildt, Iida Pullinen, Monika Springer, Einhard Kleist, Ralf Tillmann, Sebastian H. Schmitt, Cheng Wu, Thomas F. Mentel, Defeng Zhao, Donald R. Hastie, and Astrid Kiendler-Scharr
Atmos. Chem. Phys., 16, 11237–11248, https://doi.org/10.5194/acp-16-11237-2016, https://doi.org/10.5194/acp-16-11237-2016, 2016
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We investigated NOx impacts on the formation of secondary organic aerosol (SOA) mass from b-pinene and we could reveal two different mechanisms of impacts. One of them was the impact of NOx on OH that could explain increasing SOA yield with increasing NOx at low NOx conditions. The other was the suppression of new particle formation limiting the condensational sink for the SOA precursors. This effect could explain a substantial fraction of the decrease of SOA yield observed at high NOx.
Patrick Schlag, Astrid Kiendler-Scharr, Marcus Johannes Blom, Francesco Canonaco, Jeroen Sebastiaan Henzing, Marcel Moerman, André Stephan Henry Prévôt, and Rupert Holzinger
Atmos. Chem. Phys., 16, 8831–8847, https://doi.org/10.5194/acp-16-8831-2016, https://doi.org/10.5194/acp-16-8831-2016, 2016
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This work provides chemical composition data of atmospheric aerosols acquired during 1 year in the rural site of Cabauw, the Netherlands. In some periods, we found unexpected high particle mass concentrations exceeding the WHO limits. Using these composition data, we found that reducing ammonia emissions in this region would largely reduce the main aerosol component ammonium nitrate, whereas the local mitigation of the organics turned out to be difficult due to the lack of a designated source.
Bernadette Rosati, Martin Gysel, Florian Rubach, Thomas F. Mentel, Brigitta Goger, Laurent Poulain, Patrick Schlag, Pasi Miettinen, Aki Pajunoja, Annele Virtanen, Henk Klein Baltink, J. S. Bas Henzing, Johannes Größ, Gian Paolo Gobbi, Alfred Wiedensohler, Astrid Kiendler-Scharr, Stefano Decesari, Maria Cristina Facchini, Ernest Weingartner, and Urs Baltensperger
Atmos. Chem. Phys., 16, 7295–7315, https://doi.org/10.5194/acp-16-7295-2016, https://doi.org/10.5194/acp-16-7295-2016, 2016
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This study presents PEGASOS project data from field campaigns in the Po Valley, Italy and the Netherlands. Vertical profiles of aerosol hygroscopicity and chemical composition were investigated with airborne measurements on board a Zeppelin NT airship. A special focus was on the evolution of different mixing layers within the PBL as a function of daytime. A closure study showed that variations in aerosol hygroscopicity can well be explained by the variations in chemical composition.
Hendrik Fuchs, Zhaofeng Tan, Andreas Hofzumahaus, Sebastian Broch, Hans-Peter Dorn, Frank Holland, Christopher Künstler, Sebastian Gomm, Franz Rohrer, Stephanie Schrade, Ralf Tillmann, and Andreas Wahner
Atmos. Meas. Tech., 9, 1431–1447, https://doi.org/10.5194/amt-9-1431-2016, https://doi.org/10.5194/amt-9-1431-2016, 2016
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The hydroxyl radical is the key reactant that controls the chemical transformation of pollutants in the atmosphere. Observations of nighttime radicals concentrations were larger than predicted by models in field campaigns in forested and urban environments. Here, we investigated, if measurements could have been affected by artifacts. No significant interferences were found for atmospheric concentrations of reactants in ozonolysis experiments, but small artificats from nitrate radicals.
T. Hohaus, U. Kuhn, S. Andres, M. Kaminski, F. Rohrer, R. Tillmann, A. Wahner, R. Wegener, Z. Yu, and A. Kiendler-Scharr
Atmos. Meas. Tech., 9, 1247–1259, https://doi.org/10.5194/amt-9-1247-2016, https://doi.org/10.5194/amt-9-1247-2016, 2016
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As an extension of the atmosphere simulation chamber SAPHIR, an environmentally-controlled dynamic (flow-through) plant chamber under SAPHIR (SAPHIR-PLUS) was developed. This facility allows for feeding a natural blend of biogenic trace gases into SAPHIR. PLUS is utilized to characterize the atmospheric chemistry of natural trace gas mixtures at close to ambient concentration levels. In this study, the results of the initial characterization experiments are presented in detail.
Andrea Ghirardo, Junfei Xie, Xunhua Zheng, Yuesi Wang, Rüdiger Grote, Katja Block, Jürgen Wildt, Thomas Mentel, Astrid Kiendler-Scharr, Mattias Hallquist, Klaus Butterbach-Bahl, and Jörg-Peter Schnitzler
Atmos. Chem. Phys., 16, 2901–2920, https://doi.org/10.5194/acp-16-2901-2016, https://doi.org/10.5194/acp-16-2901-2016, 2016
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Trees can impact urban air quality. Large emissions of plant volatiles are emitted in Beijing as a stress response to the urban polluted environment, but their impacts on secondary particulate matter remain relatively low compared to those originated from anthropogenic activities. The present study highlights the importance of including stress-induced compounds when studying plant volatile emissions.
M. Dal Maso, L. Liao, J. Wildt, A. Kiendler-Scharr, E. Kleist, R. Tillmann, M. Sipilä, J. Hakala, K. Lehtipalo, M. Ehn, V.-M. Kerminen, M. Kulmala, D. Worsnop, and T. Mentel
Atmos. Chem. Phys., 16, 1955–1970, https://doi.org/10.5194/acp-16-1955-2016, https://doi.org/10.5194/acp-16-1955-2016, 2016
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In this paper, we present the first direct laboratory observations of nanoparticle formation from sulfuric acid and realistic BVOC precursor vapour mixtures performed at atmospherically relevant concentration levels. We found that the formation rate was proportional to the product of sulphuric acid and biogenic VOC emission strength, and that the formation rates were consistent with a mechanism in which nucleating BVOC oxidation products are rapidly formed and activate with sulfuric acid.
K.-E. Min, R. A. Washenfelder, W. P. Dubé, A. O. Langford, P. M. Edwards, K. J. Zarzana, J. Stutz, K. Lu, F. Rohrer, Y. Zhang, and S. S. Brown
Atmos. Meas. Tech., 9, 423–440, https://doi.org/10.5194/amt-9-423-2016, https://doi.org/10.5194/amt-9-423-2016, 2016
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We have developed a two-channel broadband cavity enhanced absorption spectrometer for field measurements of glyoxal, methylglyoxal, nitrous acid, nitrogen dioxide, and water. We have successfully deployed this instrument during two aircraft and two ground-based field campaigns. The demonstrated precision (2σ) for retrievals of CHOCHO, HONO, and NO2 are 34, 350, and 80 parts per trillion (pptv) in 5 s, with accuracy of 5.8, 9.0 and 5.0 %.
D. F. Zhao, A. Buchholz, B. Kortner, P. Schlag, F. Rubach, H. Fuchs, A. Kiendler-Scharr, R. Tillmann, A. Wahner, Å. K. Watne, M. Hallquist, J. M. Flores, Y. Rudich, K. Kristensen, A. M. K. Hansen, M. Glasius, I. Kourtchev, M. Kalberer, and Th. F. Mentel
Atmos. Chem. Phys., 16, 1105–1121, https://doi.org/10.5194/acp-16-1105-2016, https://doi.org/10.5194/acp-16-1105-2016, 2016
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This study investigated the cloud droplet activation behavior and hygroscopic growth of mixed anthropogenic and biogenic SOA (ABSOA) compared to pure biogenic SOA (BSOA) and pure anthropogenic SOA (ASOA). Cloud droplet activation behaviors of different types of SOA were similar. In contrast, the hygroscopicity of ASOA was higher than BSOA and ABSOA. ASOA components enhanced the hygroscopicity of the ABSOA. Yet this enhancement cannot be described by a linear mixing of pure SOA systems.
P. Roldin, L. Liao, D. Mogensen, M. Dal Maso, A. Rusanen, V.-M. Kerminen, T. F. Mentel, J. Wildt, E. Kleist, A. Kiendler-Scharr, R. Tillmann, M. Ehn, M. Kulmala, and M. Boy
Atmos. Chem. Phys., 15, 10777–10798, https://doi.org/10.5194/acp-15-10777-2015, https://doi.org/10.5194/acp-15-10777-2015, 2015
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We used the ADCHAM model to study new particle formation events in the JPAC chamber. The model results show that the new particles may be formed by a kinetic type of nucleation involving both sulphuric acid and organic compounds formed from OH oxidation of volatile organic compounds (VOCs). The observed particle growth may either be controlled by the condensation of semi- and low-volatililty organic compounds or by the formation of low-volatility compounds (oligomers) at the particle surface.
T. F. Mentel, M. Springer, M. Ehn, E. Kleist, I. Pullinen, T. Kurtén, M. Rissanen, A. Wahner, and J. Wildt
Atmos. Chem. Phys., 15, 6745–6765, https://doi.org/10.5194/acp-15-6745-2015, https://doi.org/10.5194/acp-15-6745-2015, 2015
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We studied a series of cycloalkenes and methyl-substituted alkenes in order to elucidate the structural pre-requisites and chemical pathways to the recently discovered class of highly oxidized molecules ELVOC (Ehn et al., Nature, 2014). ELVOC may totally change the view on (parts of) the mechanism of SOA formation. We present results which support recent observations of H shifts from C-H to peroxy radicals, highlighting the pivotal role of peroxyradicals in organic atmospheric chemistry.
J. Kaiser, G. M. Wolfe, B. Bohn, S. Broch, H. Fuchs, L. N. Ganzeveld, S. Gomm, R. Häseler, A. Hofzumahaus, F. Holland, J. Jäger, X. Li, I. Lohse, K. Lu, A. S. H. Prévôt, F. Rohrer, R. Wegener, R. Wolf, T. F. Mentel, A. Kiendler-Scharr, A. Wahner, and F. N. Keutsch
Atmos. Chem. Phys., 15, 1289–1298, https://doi.org/10.5194/acp-15-1289-2015, https://doi.org/10.5194/acp-15-1289-2015, 2015
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Using measurements acquired from a Zeppelin airship during the PEGASOS 2012 campaign, we show that VOC oxidation alone cannot account for the formaldehyde concentrations observed in the morning over rural Italy. Vertical profiles suggest a ground-level source of HCHO. Incorporating this additional HCHO source into a photochemical model increases calculated O3 production by as much as 12%.
D. F. Zhao, M. Kaminski, P. Schlag, H. Fuchs, I.-H. Acir, B. Bohn, R. Häseler, A. Kiendler-Scharr, F. Rohrer, R. Tillmann, M. J. Wang, R. Wegener, J. Wildt, A. Wahner, and Th. F. Mentel
Atmos. Chem. Phys., 15, 991–1012, https://doi.org/10.5194/acp-15-991-2015, https://doi.org/10.5194/acp-15-991-2015, 2015
C. Wu, I. Pullinen, S. Andres, G. Carriero, S. Fares, H. Goldbach, L. Hacker, T. Kasal, A. Kiendler-Scharr, E. Kleist, E. Paoletti, A. Wahner, J. Wildt, and Th. F. Mentel
Biogeosciences, 12, 177–191, https://doi.org/10.5194/bg-12-177-2015, https://doi.org/10.5194/bg-12-177-2015, 2015
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Impacts of soil moisture on de novo monoterpene emissions from several tree species were studied. Mild drought slightly increased MT emissions, but with further progressing drought the emissions decreased to almost zero. Increases of MT emissions were explainable by increases of leaf temperature due to lowered transpirational cooling. The decrease of emissions observed when soil moisture fell below certain thresholds was parameterized, allowing considering impacts of soil moisture in models.
H. G. J. Smit, S. Rohs, P. Neis, D. Boulanger, M. Krämer, A. Wahner, and A. Petzold
Atmos. Chem. Phys., 14, 13241–13255, https://doi.org/10.5194/acp-14-13241-2014, https://doi.org/10.5194/acp-14-13241-2014, 2014
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Long-term water vapour measurements from the MOZAIC programme are a unique source for upper troposphere humidity data. However, due to an error in the calibration procedure, RH data from MOZAIC were biased towards higher values for the period starting in year 2000. Here we report the procedures followed to reanalyse the calibrations and to reprocess the entire MOZAIC RH data. This study serves as the reference publication for the reanalysed MOZAIC RH data base for the period 1994 to 2009.
X. Li, F. Rohrer, T. Brauers, A. Hofzumahaus, K. Lu, M. Shao, Y. H. Zhang, and A. Wahner
Atmos. Chem. Phys., 14, 12291–12305, https://doi.org/10.5194/acp-14-12291-2014, https://doi.org/10.5194/acp-14-12291-2014, 2014
H. Berresheim, M. Adam, C. Monahan, C. O'Dowd, J. M. C. Plane, B. Bohn, and F. Rohrer
Atmos. Chem. Phys., 14, 12209–12223, https://doi.org/10.5194/acp-14-12209-2014, https://doi.org/10.5194/acp-14-12209-2014, 2014
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Sulfuric acid plays a major role in the formation of aerosol particles and clouds. Measurements at the west coast of Ireland reveal that oxidation of SO2 by OH explains only 20%, on average, of H2SO4 formation in coastal marine air. Additional sources may be (a) oxidation by Criegee intermediates produced photolytically and/or (b) formation from SO3 instead of SO2 in the oxidation of dimethyl sulfide, suggesting an important role of marine emissions in the self-cleaning power of the atmosphere.
R. Dlugi, M. Berger, M. Zelger, A. Hofzumahaus, F. Rohrer, F. Holland, K. Lu, and G. Kramm
Atmos. Chem. Phys., 14, 10333–10362, https://doi.org/10.5194/acp-14-10333-2014, https://doi.org/10.5194/acp-14-10333-2014, 2014
C. Fountoukis, A. G. Megaritis, K. Skyllakou, P. E. Charalampidis, C. Pilinis, H. A. C. Denier van der Gon, M. Crippa, F. Canonaco, C. Mohr, A. S. H. Prévôt, J. D. Allan, L. Poulain, T. Petäjä, P. Tiitta, S. Carbone, A. Kiendler-Scharr, E. Nemitz, C. O'Dowd, E. Swietlicki, and S. N. Pandis
Atmos. Chem. Phys., 14, 9061–9076, https://doi.org/10.5194/acp-14-9061-2014, https://doi.org/10.5194/acp-14-9061-2014, 2014
H. Fuchs, I.-H. Acir, B. Bohn, T. Brauers, H.-P. Dorn, R. Häseler, A. Hofzumahaus, F. Holland, M. Kaminski, X. Li, K. Lu, A. Lutz, S. Nehr, F. Rohrer, R. Tillmann, R. Wegener, and A. Wahner
Atmos. Chem. Phys., 14, 7895–7908, https://doi.org/10.5194/acp-14-7895-2014, https://doi.org/10.5194/acp-14-7895-2014, 2014
S. Nehr, B. Bohn, H.-P. Dorn, H. Fuchs, R. Häseler, A. Hofzumahaus, X. Li, F. Rohrer, R. Tillmann, and A. Wahner
Atmos. Chem. Phys., 14, 6941–6952, https://doi.org/10.5194/acp-14-6941-2014, https://doi.org/10.5194/acp-14-6941-2014, 2014
M. Crippa, F. Canonaco, V. A. Lanz, M. Äijälä, J. D. Allan, S. Carbone, G. Capes, D. Ceburnis, M. Dall'Osto, D. A. Day, P. F. DeCarlo, M. Ehn, A. Eriksson, E. Freney, L. Hildebrandt Ruiz, R. Hillamo, J. L. Jimenez, H. Junninen, A. Kiendler-Scharr, A.-M. Kortelainen, M. Kulmala, A. Laaksonen, A. A. Mensah, C. Mohr, E. Nemitz, C. O'Dowd, J. Ovadnevaite, S. N. Pandis, T. Petäjä, L. Poulain, S. Saarikoski, K. Sellegri, E. Swietlicki, P. Tiitta, D. R. Worsnop, U. Baltensperger, and A. S. H. Prévôt
Atmos. Chem. Phys., 14, 6159–6176, https://doi.org/10.5194/acp-14-6159-2014, https://doi.org/10.5194/acp-14-6159-2014, 2014
J. M. Flores, D. F. Zhao, L. Segev, P. Schlag, A. Kiendler-Scharr, H. Fuchs, Å. K. Watne, N. Bluvshtein, Th. F. Mentel, M. Hallquist, and Y. Rudich
Atmos. Chem. Phys., 14, 5793–5806, https://doi.org/10.5194/acp-14-5793-2014, https://doi.org/10.5194/acp-14-5793-2014, 2014
J. Kaiser, X. Li, R. Tillmann, I. Acir, F. Holland, F. Rohrer, R. Wegener, and F. N. Keutsch
Atmos. Meas. Tech., 7, 1571–1580, https://doi.org/10.5194/amt-7-1571-2014, https://doi.org/10.5194/amt-7-1571-2014, 2014
K. D. Lu, F. Rohrer, F. Holland, H. Fuchs, T. Brauers, A. Oebel, R. Dlugi, M. Hu, X. Li, S. R. Lou, M. Shao, T. Zhu, A. Wahner, Y. H. Zhang, and A. Hofzumahaus
Atmos. Chem. Phys., 14, 4979–4999, https://doi.org/10.5194/acp-14-4979-2014, https://doi.org/10.5194/acp-14-4979-2014, 2014
J. Wildt, T. F. Mentel, A. Kiendler-Scharr, T. Hoffmann, S. Andres, M. Ehn, E. Kleist, P. Müsgen, F. Rohrer, Y. Rudich, M. Springer, R. Tillmann, and A. Wahner
Atmos. Chem. Phys., 14, 2789–2804, https://doi.org/10.5194/acp-14-2789-2014, https://doi.org/10.5194/acp-14-2789-2014, 2014
M. Paglione, A. Kiendler-Scharr, A. A. Mensah, E. Finessi, L. Giulianelli, S. Sandrini, M. C. Facchini, S. Fuzzi, P. Schlag, A. Piazzalunga, E. Tagliavini, J. S. Henzing, and S. Decesari
Atmos. Chem. Phys., 14, 25–45, https://doi.org/10.5194/acp-14-25-2014, https://doi.org/10.5194/acp-14-25-2014, 2014
R. M. Varma, S. M. Ball, T. Brauers, H.-P. Dorn, U. Heitmann, R. L. Jones, U. Platt, D. Pöhler, A. A. Ruth, A. J. L. Shillings, J. Thieser, A. Wahner, and D. S. Venables
Atmos. Meas. Tech., 6, 3115–3130, https://doi.org/10.5194/amt-6-3115-2013, https://doi.org/10.5194/amt-6-3115-2013, 2013
Th. F. Mentel, E. Kleist, S. Andres, M. Dal Maso, T. Hohaus, A. Kiendler-Scharr, Y. Rudich, M. Springer, R. Tillmann, R. Uerlings, A. Wahner, and J. Wildt
Atmos. Chem. Phys., 13, 8755–8770, https://doi.org/10.5194/acp-13-8755-2013, https://doi.org/10.5194/acp-13-8755-2013, 2013
Y. P. Li, H. Elbern, K. D. Lu, E. Friese, A. Kiendler-Scharr, Th. F. Mentel, X. S. Wang, A. Wahner, and Y. H. Zhang
Atmos. Chem. Phys., 13, 6289–6304, https://doi.org/10.5194/acp-13-6289-2013, https://doi.org/10.5194/acp-13-6289-2013, 2013
H.-P. Dorn, R. L. Apodaca, S. M. Ball, T. Brauers, S. S. Brown, J. N. Crowley, W. P. Dubé, H. Fuchs, R. Häseler, U. Heitmann, R. L. Jones, A. Kiendler-Scharr, I. Labazan, J. M. Langridge, J. Meinen, T. F. Mentel, U. Platt, D. Pöhler, F. Rohrer, A. A. Ruth, E. Schlosser, G. Schuster, A. J. L. Shillings, W. R. Simpson, J. Thieser, R. Tillmann, R. Varma, D. S. Venables, and A. Wahner
Atmos. Meas. Tech., 6, 1111–1140, https://doi.org/10.5194/amt-6-1111-2013, https://doi.org/10.5194/amt-6-1111-2013, 2013
E. U. Emanuelsson, M. Hallquist, K. Kristensen, M. Glasius, B. Bohn, H. Fuchs, B. Kammer, A. Kiendler-Scharr, S. Nehr, F. Rubach, R. Tillmann, A. Wahner, H.-C. Wu, and Th. F. Mentel
Atmos. Chem. Phys., 13, 2837–2855, https://doi.org/10.5194/acp-13-2837-2013, https://doi.org/10.5194/acp-13-2837-2013, 2013
E. Kleist, T. F. Mentel, S. Andres, A. Bohne, A. Folkers, A. Kiendler-Scharr, Y. Rudich, M. Springer, R. Tillmann, and J. Wildt
Biogeosciences, 9, 5111–5123, https://doi.org/10.5194/bg-9-5111-2012, https://doi.org/10.5194/bg-9-5111-2012, 2012
Related subject area
Subject: Gases | Technique: In Situ Measurement | Topic: Validation and Intercomparisons
Improving consistency in methane emission quantification from the natural gas distribution systems across measurement devices
Interpretation of mass spectra by a Vocus proton-transfer-reaction mass spectrometer (PTR-MS) at an urban site: insights from gas chromatographic pre-separation
Improving the quantification of peak concentrations for air quality sensors via data weighting
Long-term observations of atmospheric CO2 and CH4 trends and comparison of two measurement systems at Pallas-Sammaltunturi station in Northern Finland
Evaluating mass flow meter measurements from chambers for greenhouse gas emission from orphan wells and other point sources
An evaluation of airborne mass balance and tracer correlation approaches to estimate site-level CH4 emissions from LNG facilities using CO2 as a tracer of opportunity
Calibrating adsorptive and reactive losses of monoterpenes and sesquiterpenes in dynamic chambers using deuterated surrogates
Orphaned Oil & Gas Well Methane Emission Rates Quantified with Gaussian Plume Inversions of Ambient Observations
OF–CEAS laser spectroscopy to measure water isotopes in dry environments: example of application in Antarctica
Performance evaluation of air quality sensors for environmental epidemiology
Towards a high-quality in situ observation network for oxygenated volatile organic compounds (OVOCs) in Europe: transferring metrological traceability to the field
Intercomparison of IAGOS-CORE, IAGOS-CARIBIC and WMO/GAW-WCCOS Ozone Instruments at the Environmental Simulation Facility at Jülich, Germany
Validation of formaldehyde products from three satellite retrievals (OMI SAO, OMPS-NPP SAO, and OMI BIRA) in the marine atmosphere with four seasons of Atmospheric Tomography Mission (ATom) aircraft observations
Methodology and uncertainty estimation for measurements of methane leakage in a manufactured house
Evaluating Weather and Chemical Transport Models at High Latitudes using MAGIC2021 Airborne Measurements
Alternate materials for the capture and quantification of gaseous oxidized mercury in the atmosphere
Lower-cost eddy covariance for CO2 and H2O fluxes over grassland and agroforestry
Evaluation of optimized flux chamber design for measurement of ammonia emission after field application of slurry with full-scale farm machinery
Preparation of low-concentration H2 test gas mixtures in ambient air for calibration of H2 sensors
Pico-Light H2O: intercomparison of in situ water vapour measurements during the AsA 2022 campaign
Mobile air quality monitoring and comparison to fixed monitoring sites for instrument performance assessment
Intercomparison of eddy-covariance software for urban tall-tower sites
Assessment of current methane emission quantification techniques for natural gas midstream applications
Performance assessment of state-of-the-art and novel methods for remote compliance monitoring of sulfur emissions from shipping
Intercomparison of detection and quantification methods for methane emissions from the natural gas distribution network in Hamburg, Germany
Comparison of photoacoustic spectroscopy and cavity ring-down spectroscopy for ambient methane monitoring at Hohenpeißenberg
Comparison of atmospheric CO, CO2 and CH4 measurements at the Schneefernerhaus and the mountain ridge at Zugspitze
Intercomparison of commercial analyzers for atmospheric ethane and methane observations
Real-time measurement of phase partitioning of organic compounds using a proton-transfer-reaction time-of-flight mass spectrometer coupled to a CHARON inlet
A quantitative comparison of methods used to measure smaller methane emissions typically observed from superannuated oil and gas infrastructure
Comparing airborne algorithms for greenhouse gas flux measurements over the Alberta oil sands
Characterization of inexpensive metal oxide sensor performance for trace methane detection
Intercomparison of upper tropospheric and lower stratospheric water vapor measurements over the Asian Summer Monsoon during the StratoClim campaign
Air pollution measurement errors: is your data fit for purpose?
Performance characterization of low-cost air quality sensors for off-grid deployment in rural Malawi
Comment on “Comparison of ozone measurement methods in biomass burning smoke: an evaluation under field and laboratory conditions” by Long et al. (2021)
Homogenization of the Observatoire de Haute Provence electrochemical concentration cell (ECC) ozonesonde data record: comparison with lidar and satellite observations
Long-term behavior and stability of calibration models for NO and NO2 low-cost sensors
Controlled-release experiment to investigate uncertainties in UAV-based emission quantification for methane point sources
Ozone formation sensitivity study using machine learning coupled with the reactivity of volatile organic compound species
Evaluating uncertainty in sensor networks for urban air pollution insights
Estimating oil sands emissions using horizontal path-integrated column measurements
Global evaluation of the precipitable-water-vapor product from MERSI-II (Medium Resolution Spectral Imager) on board the Fengyun-3D satellite
Field testing two flux footprint models
Validation of a new cavity ring-down spectrometer for measuring tropospheric gaseous hydrogen chloride
A field intercomparison of three passive air samplers for gaseous mercury in ambient air
Beef cattle methane emissions measured with tracer-ratio and inverse dispersion modelling techniques
Methane emissions from an oil sands tailings pond: a quantitative comparison of fluxes derived by different methods
Performance of open-path GasFinder3 devices for CH4 concentration measurements close to ambient levels
Water vapor density and turbulent fluxes from three generations of infrared gas analyzers
Judith Tettenborn, Daniel Zavala-Araiza, Daan Stroeken, Hossein Maazallahi, Carina van der Veen, Arjan Hensen, Ilona Velzeboer, Pim van den Bulk, Felix Vogel, Lawson Gillespie, Sebastien Ars, James France, David Lowry, Rebecca Fisher, and Thomas Röckmann
Atmos. Meas. Tech., 18, 3569–3584, https://doi.org/10.5194/amt-18-3569-2025, https://doi.org/10.5194/amt-18-3569-2025, 2025
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Measurements of methane with vehicle-based sensors are an effective method to identify and quantify leaks from urban gas distribution systems. We deliberately released methane in different environments and calibrated the response of different methane analysers when they transected the plumes in a vehicle. We derived an improved statistical function for consistent emission estimations using different instruments. Repeated transects reduce the uncertainty in emission rate estimates.
Ying Zhang, Yuwei Wang, Chuang Li, Yueyang Li, Sijia Yin, Megan S. Claflin, Brian M. Lerner, Douglas Worsnop, and Lin Wang
Atmos. Meas. Tech., 18, 3547–3568, https://doi.org/10.5194/amt-18-3547-2025, https://doi.org/10.5194/amt-18-3547-2025, 2025
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This study provides insight into how individual ions measured by proton-transfer-reaction (PTR) mass spectrometry are produced by multiple volatile organic compounds (VOCs). A reference table is provided for attributing the PTR signal to contributing VOC species. The signals are grouped according to the complexity of their potential identities. We find that a number of signal ions such as C6H7+ for benzene and C5H9+ for isoprene merely give an upper limit of their corresponding concentrations.
Caroline Frischmon, Jonathan Silberstein, Annamarie Guth, Erick Mattson, Jack Porter, and Michael Hannigan
Atmos. Meas. Tech., 18, 3147–3159, https://doi.org/10.5194/amt-18-3147-2025, https://doi.org/10.5194/amt-18-3147-2025, 2025
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Air quality sensors often underpredict peak concentrations, which is a major issue in applications such as emission event detection. Here, we detail a novel approach involving data weighting to improve quantification of these peak values. To demonstrate its effectiveness, we applied data weighting to carbon monoxide, methane, and volatile organic compound sensor data. This work broadens our ability to use air sensors in contexts where accurate quantification of peak concentrations is essential.
Antti Laitinen, Hermanni Aaltonen, Christoph Zellweger, Aki Tsuruta, Tuula Aalto, and Juha Hatakka
Atmos. Meas. Tech., 18, 3109–3133, https://doi.org/10.5194/amt-18-3109-2025, https://doi.org/10.5194/amt-18-3109-2025, 2025
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This paper presents long-term observations of atmospheric CO2 and CH4 mole fractions and a comparison of two permanent and two mobile measurement systems located in Northern Finland. Furthermore, the observed mole fractions are compared against the mean marine boundary layer product for the Northern Hemisphere. The comparisons of all the systems show good agreement in relation to the World Meteorological Organization/Global Atmosphere Watch network compatibility goal limits for CO2 and CH4.
Karl B. Haase and Nicholas J. Gianoutsos
EGUsphere, https://doi.org/10.5194/egusphere-2025-1201, https://doi.org/10.5194/egusphere-2025-1201, 2025
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This work demonstrates a simple approach for using mass flow meters connected to rigid chambers for measuring gas emissions rates in situations the meter cannot be attached directly, such as orphan oil and gas wells. This paper shows the results of performance testing, demonstrates common sources of uncertainty, and provides suggestions for how to use the approach to generate the best quality data. The findings can be used by researchers, the petroleum industry, regulators, and carbon markets.
Mark F. Lunt, Stephen J. Harris, Jorg Hacker, Ian Joynes, Tim Robertson, Simon Thompson, and James L. France
EGUsphere, https://doi.org/10.5194/egusphere-2025-1926, https://doi.org/10.5194/egusphere-2025-1926, 2025
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To ensure robust use of measurement-based approaches to estimate methane emissions from individual sites, it is important to validate the accuracy of the methods used in the field. By using co-emitted carbon dioxide, we evaluate the performance of one such quantification method at liquefied natural gas terminals. We further demonstrate the potential for a more efficient quantification approach by considering the ratio of methane to carbon dioxide concentrations.
Jianqiang Zeng, Yanli Zhang, Haofan Ran, Weihua Pang, Hao Guo, Zhaobin Mu, Wei Song, and Xinming Wang
Atmos. Meas. Tech., 18, 1811–1821, https://doi.org/10.5194/amt-18-1811-2025, https://doi.org/10.5194/amt-18-1811-2025, 2025
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This study revealed the existence of significant species-specific adsorptive and reactive losses of monoterpenes and sesquiterpenes in dynamic chambers. The deuterated α-pinene-d3 and β-caryophyllene-d2 were proven as effective surrogates in tracing these losses for some key monoterpenes and sesquiterpenes. The findings highlight the importance of selecting internal surrogates that closely match the adsorptive and reactive behaviors of target compounds for precise loss correction.
Emily Follansbee, James E. Lee, Mohit L. Dubey, Jonathan F. Dooley, Curtis Shuck, Ken Minschwaner, Andre Santos, Sebastien C. Biraud, and Manvendra K. Dubey
EGUsphere, https://doi.org/10.5194/egusphere-2025-344, https://doi.org/10.5194/egusphere-2025-344, 2025
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This work uses ambient methane and wind measurements to quantify methane emissions from a leaking orphaned oil and gas well using Gaussian plume inversions. Our analysis shows that existing Gaussian plume methods that assume atmospheric stability are prone to large errors. We report a more robust analysis that determines plume dispersion coefficients from our in situ observations. Our technique enables more accurate methane quantification of orphaned oil and gas wells to prioritize plugging.
Thomas Lauwers, Elise Fourré, Olivier Jossoud, Daniele Romanini, Frédéric Prié, Giordano Nitti, Mathieu Casado, Kévin Jaulin, Markus Miltner, Morgane Farradèche, Valérie Masson-Delmotte, and Amaëlle Landais
Atmos. Meas. Tech., 18, 1135–1147, https://doi.org/10.5194/amt-18-1135-2025, https://doi.org/10.5194/amt-18-1135-2025, 2025
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Water vapour isotopes are important tools to better understand processes governing the atmospheric hydrological cycle. In polar regions, their measurement helps to improve the interpretation of water isotopic records in ice cores. However, in situ water vapour isotopic monitoring is an important challenge, especially in dry places of East Antarctica. We present here an alternative laser spectroscopy technique adapted for such measurements, with a limit of detection down to 10 ppm humidity.
Miriam Chacón-Mateos, Héctor García-Salamero, Bernd Laquai, and Ulrich Vogt
EGUsphere, https://doi.org/10.5194/egusphere-2025-587, https://doi.org/10.5194/egusphere-2025-587, 2025
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This study evaluates air quality sensors in indoor & outdoor environments to support health research. Sensors were calibrated using data from reference instruments, and regression and machine learning models were tested for data correction. Results highlight the importance of using high-quality training data during co-location. Integrating metadata, such as activity logs, helps validate calibrated sensor data. These findings can enhance the use of air quality sensors in health studies globally.
Maitane Iturrate-Garcia, Thérèse Salameh, Paul Schlauri, Annarita Baldan, Martin K. Vollmer, Evdokia Stratigou, Sebastien Dusanter, Jianrong Li, Stefan Persijn, Anja Claude, Rupert Holzinger, Christophe Sutour, Tatiana Macé, Yasin Elshorbany, Andreas Ackermann, Céline Pascale, and Stefan Reimann
Atmos. Meas. Tech., 18, 371–403, https://doi.org/10.5194/amt-18-371-2025, https://doi.org/10.5194/amt-18-371-2025, 2025
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Accurate and comparable measurements of oxygenated organic compounds (OVOCs) are crucial in assessing tropospheric ozone burdens and trends. However, the monitoring of many OVOCs remains challenging because of their low atmospheric abundance and lack of stable and traceable calibration standards. This paper describes the calibration standards developed for OVOCs at a low amount of substance fractions (<100 nmol mol-1) to transfer traceability of the International System of Units to the field.
Herman G.J. Smit, Torben Galle, Romain Blot, Florian Obersteiner, Philippe Nédélec, Andreas Zahn, Jean-Marc Cousin, Ulrich Bundke, Andreas Petzold, Valerie Thouret, and Hannah Clark
EGUsphere, https://doi.org/10.5194/egusphere-2024-3760, https://doi.org/10.5194/egusphere-2024-3760, 2025
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The two ozone instruments of IAGOS (In-service Aircraft for a Global Observation System) have been compared with the Ozone PhotoMeter (OPM) of the World Calibration Center of Ozone Sondes (WCCOS) in an atmospheric simulation chamber under realistic flight conditions of pressure, temperature, and ozone concentrations. The two IAGOS-instruments showed good agreement with the OPM within 5–6 %. The observed differences are small but systematic and reproducible during the intercomparison.
Jin Liao, Glenn M. Wolfe, Alexander E. Kotsakis, Julie M. Nicely, Jason M. St. Clair, Thomas F. Hanisco, Gonzalo González Abad, Caroline R. Nowlan, Zolal Ayazpour, Isabelle De Smedt, Eric C. Apel, and Rebecca S. Hornbrook
Atmos. Meas. Tech., 18, 1–16, https://doi.org/10.5194/amt-18-1-2025, https://doi.org/10.5194/amt-18-1-2025, 2025
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Validation of satellite HCHO over the remote marine regions is relatively low, and modeled HCHO in these regions is usually added as a global satellite HCHO background. This paper intercompares three satellite HCHO retrievals and validates them against in situ observations from the NASA ATom mission. All retrievals are correlated with ATom-integrated columns over remote oceans, with OMI SAO (v004) showing the best agreement. A persistent low bias is found in all retrievals at high latitudes.
Anna Karion, Michael F. Link, Rileigh Robertson, Tyler Boyle, and Dustin Poppendieck
Atmos. Meas. Tech., 17, 7065–7075, https://doi.org/10.5194/amt-17-7065-2024, https://doi.org/10.5194/amt-17-7065-2024, 2024
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Methane leaks into houses that use natural gas from appliances, pipes, and fittings. We measured methane emitted from a manufactured house under different ventilation conditions using indoor and outdoor concentration measurements. We injected methane at prescribed rates into the house and then measured the emissions using our method. We report the error in the calculation based on these tests. We also describe the method and provide guidance on conducting this type of experiment.
Félix Langot, Cyril Crevoisier, Thomas Lauvaux, Charbel Abdallah, Jérôme Pernin, Xin Lin, Marielle Saunois, Axel Guedj, Thomas Ponthieu, Anke Roiger, Klaus-Dirk Gottschaldt, and Alina Fiehn
EGUsphere, https://doi.org/10.5194/egusphere-2024-3559, https://doi.org/10.5194/egusphere-2024-3559, 2024
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Our study compares outputs from meteorological and atmospheric composition models to data from the MAGIC2021 campaign that took place in Sweden. Our results highlight performance differences among models, revealing strengths and weaknesses of different modelling techniques. We also found that wetland emission inventories overestimated emissions in regional simulations. This work helps refining methane emission predictions, essential for understanding climate change.
Livia Lown, Sarrah M. Dunham-Cheatham, Seth N. Lyman, and Mae S. Gustin
Atmos. Meas. Tech., 17, 6397–6413, https://doi.org/10.5194/amt-17-6397-2024, https://doi.org/10.5194/amt-17-6397-2024, 2024
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New sorbent materials are needed to preconcentrate atmospheric oxidized mercury for analysis by developing mass spectrometry methods. Chitosan, α-Al2O3, and γ-Al2O3 were tested for quantitative gaseous oxidized mercury sorption in ambient air under laboratory and field conditions. Although these materials sorbed gaseous oxidized mercury without sorbing elemental mercury in the laboratory, less oxidized mercury was recovered from these materials compared to cation exchange membranes in the field.
Justus G. V. van Ramshorst, Alexander Knohl, José Ángel Callejas-Rodelas, Robert Clement, Timothy C. Hill, Lukas Siebicke, and Christian Markwitz
Atmos. Meas. Tech., 17, 6047–6071, https://doi.org/10.5194/amt-17-6047-2024, https://doi.org/10.5194/amt-17-6047-2024, 2024
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In this work we present experimental field results of a lower-cost eddy covariance (LC-EC) system, which can measure the ecosystem exchange of carbon dioxide and water vapour with the atmosphere. During three field campaigns on a grassland and agroforestry grassland, we compared the LC-EC with a conventional eddy covariance (CON-EC) system. Our results show that LC-EC has the potential to measure EC fluxes at only approximately 25 % of the cost of a CON-EC system.
Johanna Pedersen, Sasha D. Hafner, Andreas Pacholski, Valthor I. Karlsson, Li Rong, Rodrigo Labouriau, and Jesper N. Kamp
Atmos. Meas. Tech., 17, 4493–4505, https://doi.org/10.5194/amt-17-4493-2024, https://doi.org/10.5194/amt-17-4493-2024, 2024
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Field-applied animal slurry is a significant source of NH3 emission. A new system of dynamic flux chambers for NH3 measurements was developed and validated using three field trials in order to assess the variability after application with a trailing hose at different scales: manual (handheld) application, a 3 m slurry boom, and a 30 m slurry boom. The system facilitates NH3 emission measurement with replication after both manual and farm-scale slurry application with relatively high precision.
Niklas Karbach, Lisa Höhler, Peter Hoor, Heiko Bozem, Nicole Bobrowski, and Thorsten Hoffmann
Atmos. Meas. Tech., 17, 4081–4086, https://doi.org/10.5194/amt-17-4081-2024, https://doi.org/10.5194/amt-17-4081-2024, 2024
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The system presented here can accurately generate and reproduce a stable flow of gas mixtures of known concentrations over several days using ambient air as a dilution medium. In combination with the small size and low weight of the system, this enables the calibration of hydrogen sensors in the field, reducing the influence of matrix effects on the accuracy of the sensor. The system is inexpensive to assemble and easy to maintain, which is the key to reliable measurement results.
Mélanie Ghysels, Georges Durry, Nadir Amarouche, Dale Hurst, Emrys Hall, Kensy Xiong, Jean-Charles Dupont, Jean-Christophe Samake, Fabien Frérot, Raghed Bejjani, and Emmanuel D. Riviere
Atmos. Meas. Tech., 17, 3495–3513, https://doi.org/10.5194/amt-17-3495-2024, https://doi.org/10.5194/amt-17-3495-2024, 2024
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A tunable diode laser hygrometer, “Pico-Light H2O”, is presented and its performances are evaluated during the AsA 2022 balloon-borne intercomparison campaign from Aire-sur-l'Adour (France) in September 2022. A total of 15 balloons were launched within the framework of the EU-funded HEMERA project. Pico-Light H2O has been compared in situ with the NOAA Frost Point Hygrometer in the upper troposphere and stratosphere, as well as with meteorological sondes (iMet-4 and M20) in the troposphere.
Andrew R. Whitehill, Melissa Lunden, Brian LaFranchi, Surender Kaushik, and Paul A. Solomon
Atmos. Meas. Tech., 17, 2991–3009, https://doi.org/10.5194/amt-17-2991-2024, https://doi.org/10.5194/amt-17-2991-2024, 2024
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We present an analysis from two large-scale mobile air quality monitoring campaigns in Colorado and California. We compare mobile measurements of air quality to measurements from nearby regulatory sites. The goal of this paper is to explore how fixed-site measurements (such as regulatory site measurements) can be used for ongoing instrument performance assessment of mobile monitoring platforms over extended measurement campaigns.
Changxing Lan, Matthias Mauder, Stavros Stagakis, Benjamin Loubet, Claudio D'Onofrio, Stefan Metzger, David Durden, and Pedro-Henrique Herig-Coimbra
Atmos. Meas. Tech., 17, 2649–2669, https://doi.org/10.5194/amt-17-2649-2024, https://doi.org/10.5194/amt-17-2649-2024, 2024
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Using eddy-covariance systems deployed in three cities, we aimed to elucidate the sources of discrepancies in flux estimations from different software packages. One crucial finding is the impact of low-frequency spectral loss corrections on tall-tower flux estimations. Our findings emphasize the significance of a standardized measurement setup and consistent postprocessing configurations in minimizing the systematic flux uncertainty resulting from the usage of different software packages.
Yunsong Liu, Jean-Daniel Paris, Gregoire Broquet, Violeta Bescós Roy, Tania Meixus Fernandez, Rasmus Andersen, Andrés Russu Berlanga, Emil Christensen, Yann Courtois, Sebastian Dominok, Corentin Dussenne, Travis Eckert, Andrew Finlayson, Aurora Fernández de la Fuente, Catlin Gunn, Ram Hashmonay, Juliano Grigoleto Hayashi, Jonathan Helmore, Soeren Honsel, Fabrizio Innocenti, Matti Irjala, Torgrim Log, Cristina Lopez, Francisco Cortés Martínez, Jonathan Martinez, Adrien Massardier, Helle Gottschalk Nygaard, Paula Agregan Reboredo, Elodie Rousset, Axel Scherello, Matthias Ulbricht, Damien Weidmann, Oliver Williams, Nigel Yarrow, Murès Zarea, Robert Ziegler, Jean Sciare, Mihalis Vrekoussis, and Philippe Bousquet
Atmos. Meas. Tech., 17, 1633–1649, https://doi.org/10.5194/amt-17-1633-2024, https://doi.org/10.5194/amt-17-1633-2024, 2024
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We investigated the performance of 10 methane emission quantification techniques in a blind controlled-release experiment at an inerted natural gas compressor station. We reported their respective strengths, weaknesses, and potential complementarity depending on the emission rates and atmospheric conditions. Additionally, we assess the dependence of emission quantification performance on key parameters such as wind speed, deployment constraints, and measurement duration.
Jörg Beecken, Andreas Weigelt, Simone Griesel, Johan Mellqvist, Alexander V. Conde Jacobo, Daniëlle van Dinther, Jan Duyzer, Jon Knudsen, Bettina Knudsen, and Leonidas Ntziachristos
Atmos. Meas. Tech., 16, 5883–5895, https://doi.org/10.5194/amt-16-5883-2023, https://doi.org/10.5194/amt-16-5883-2023, 2023
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Air pollution from shipping is a debated topic in science and politics. We compare different monitoring systems currently used in different European countries for the enforcement of emission limits regarding air pollution from ships according to regulation. The system performances were individually assessed in the field by comparison with true values. Non-compliant vessels with actual fuel sulfur contents > 0.15–0.19 % Sm/m can be detected by the compared systems with 95 % confidence.
Hossein Maazallahi, Antonio Delre, Charlotte Scheutz, Anders M. Fredenslund, Stefan Schwietzke, Hugo Denier van der Gon, and Thomas Röckmann
Atmos. Meas. Tech., 16, 5051–5073, https://doi.org/10.5194/amt-16-5051-2023, https://doi.org/10.5194/amt-16-5051-2023, 2023
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Measurement methods are increasingly deployed to verify reported methane emissions of gas leaks. This study describes unique advantages and limitations of three methods. Two methods are rapidly deployed, but uncertainties and biases exist for some leak locations. In contrast, the suction method could accurately determine leak rates in principle. However, this method, which provides data for the German emission inventory, creates an overall low bias in our study due to non-random site selection.
Max Müller, Stefan Weigl, Jennifer Müller-Williams, Matthias Lindauer, Thomas Rück, Simon Jobst, Rudolf Bierl, and Frank-Michael Matysik
Atmos. Meas. Tech., 16, 4263–4270, https://doi.org/10.5194/amt-16-4263-2023, https://doi.org/10.5194/amt-16-4263-2023, 2023
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Over a period of 5 d, a photoacoustic methane sensor was compared with a Picarro cavity ring-down (G2301) spectrometer. Both devices measured the ambient methane concentration at the meteorological observatory Hohenpeißenberg. Cross-sensitivities on the photoacoustic signal, due to fluctuating ambient humidity, were compensated by applying the CoNRad algorithm. The results show that photoacoustic sensors have the potential for accurate and precise greenhouse gas monitoring.
Antje Hoheisel, Cedric Couret, Bryan Hellack, and Martina Schmidt
Atmos. Meas. Tech., 16, 2399–2413, https://doi.org/10.5194/amt-16-2399-2023, https://doi.org/10.5194/amt-16-2399-2023, 2023
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High-precision CO2, CH4 and CO measurements have been carried out at Zugspitze for decades. New technologies make it possible to analyse these gases with high temporal resolution. This allows the detection of local pollution. To this end, measurements have been performed on the mountain ridge (ZGR) and are compared to routine measurements at the Schneefernerhaus (ZSF). Careful manual flagging of pollution events in the ZSF data leads to consistency with the little influenced ZGR time series.
Róisín Commane, Andrew Hallward-Driemeier, and Lee T. Murray
Atmos. Meas. Tech., 16, 1431–1441, https://doi.org/10.5194/amt-16-1431-2023, https://doi.org/10.5194/amt-16-1431-2023, 2023
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Methane / ethane ratios can be used to identify and partition the different sources of methane, especially in areas with natural gas mixed with biogenic methane emissions, such as cities. We tested three commercially available laser-based analyzers for sensitivity, precision, size, power requirement, ease of use on mobile platforms, and expertise needed to operate the instrument, and we make recommendations for use in various situations.
Yarong Peng, Hongli Wang, Yaqin Gao, Shengao Jing, Shuhui Zhu, Dandan Huang, Peizhi Hao, Shengrong Lou, Tiantao Cheng, Cheng Huang, and Xuan Zhang
Atmos. Meas. Tech., 16, 15–28, https://doi.org/10.5194/amt-16-15-2023, https://doi.org/10.5194/amt-16-15-2023, 2023
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This work examined the phase partitioning behaviors of organic compounds at hourly resolution in ambient conditions with the use of the CHemical Analysis of aeRosols ONline (CHARON) inlet coupled to a proton-transfer-reaction time-of-flight mass spectrometer (PTR-ToF-MS). Properly accounting for the neutral losses of small moieties during the molecular feature extraction from PTR mass spectra could significantly reduce uncertainties associated with the gas–particle partitioning measurements.
Stuart N. Riddick, Riley Ancona, Mercy Mbua, Clay S. Bell, Aidan Duggan, Timothy L. Vaughn, Kristine Bennett, and Daniel J. Zimmerle
Atmos. Meas. Tech., 15, 6285–6296, https://doi.org/10.5194/amt-15-6285-2022, https://doi.org/10.5194/amt-15-6285-2022, 2022
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This describes controlled release experiments at the METEC facility in Fort Collins, USA, that investigates the accuracy and precision of five methods commonly used to measure methane emissions. Methods include static/dynamic chambers, hi flow sampling, a backward Lagrangian stochastic method, and a Gaussian plume method. This is the first time that methods for measuring CH4 emissions from point sources less than 200 g CH4 h−1 have been quantitively assessed against references and each other.
Broghan M. Erland, Cristen Adams, Andrea Darlington, Mackenzie L. Smith, Andrew K. Thorpe, Gregory R. Wentworth, Steve Conley, John Liggio, Shao-Meng Li, Charles E. Miller, and John A. Gamon
Atmos. Meas. Tech., 15, 5841–5859, https://doi.org/10.5194/amt-15-5841-2022, https://doi.org/10.5194/amt-15-5841-2022, 2022
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Accurately estimating greenhouse gas (GHG) emissions is essential to reaching net-zero goals to combat the climate crisis. Airborne box-flights are ideal for assessing regional GHG emissions, as they can attain small error. We compare two box-flight algorithms and found they produce similar results, but daily variability must be considered when deriving emissions inventories. Increasing the consistency and agreement between airborne methods moves us closer to achieving more accurate estimates.
Daniel Furuta, Tofigh Sayahi, Jinsheng Li, Bruce Wilson, Albert A. Presto, and Jiayu Li
Atmos. Meas. Tech., 15, 5117–5128, https://doi.org/10.5194/amt-15-5117-2022, https://doi.org/10.5194/amt-15-5117-2022, 2022
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Methane is a major greenhouse gas and contributor to climate change with various human-caused and natural sources. Currently, atmospheric methane is expensive to sense. We investigate repurposing cheap methane safety sensors for atmospheric sensing, finding several promising sensors and identifying some of the challenges in this approach. This work will help in developing inexpensive sensor networks for methane monitoring, which will aid in reducing methane leaks and emissions.
Clare E. Singer, Benjamin W. Clouser, Sergey M. Khaykin, Martina Krämer, Francesco Cairo, Thomas Peter, Alexey Lykov, Christian Rolf, Nicole Spelten, Armin Afchine, Simone Brunamonti, and Elisabeth J. Moyer
Atmos. Meas. Tech., 15, 4767–4783, https://doi.org/10.5194/amt-15-4767-2022, https://doi.org/10.5194/amt-15-4767-2022, 2022
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In situ measurements of water vapor in the upper troposphere are necessary to study cloud formation and hydration of the stratosphere but challenging due to cold–dry conditions. We compare measurements from three water vapor instruments from the StratoClim campaign in 2017. In clear sky (clouds), point-by-point differences were <1.5±8 % (<1±8 %). This excellent agreement allows detection of fine-scale structures required to understand the impact of convection on stratospheric water vapor.
Sebastian Diez, Stuart E. Lacy, Thomas J. Bannan, Michael Flynn, Tom Gardiner, David Harrison, Nicholas Marsden, Nicholas A. Martin, Katie Read, and Pete M. Edwards
Atmos. Meas. Tech., 15, 4091–4105, https://doi.org/10.5194/amt-15-4091-2022, https://doi.org/10.5194/amt-15-4091-2022, 2022
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Regardless of the cost of the measuring instrument, there are no perfect measurements. For this reason, we compare the quality of the information provided by cheap devices when they are used to measure air pollutants and we try to emphasise that before judging the potential usefulness of the devices, the user must specify his own needs. Since commonly used performance indices/metrics can be misleading in qualifying this, we propose complementary visual analysis to the more commonly used metrics.
Ashley S. Bittner, Eben S. Cross, David H. Hagan, Carl Malings, Eric Lipsky, and Andrew P. Grieshop
Atmos. Meas. Tech., 15, 3353–3376, https://doi.org/10.5194/amt-15-3353-2022, https://doi.org/10.5194/amt-15-3353-2022, 2022
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We present findings from a 1-year pilot deployment of low-cost integrated air quality sensor packages in rural Malawi using calibration models developed during collocation with US regulatory monitors. We compare the results with data from remote sensing products and previous field studies. We conclude that while the remote calibration approach can help extract useful data, great care is needed when assessing low-cost sensor data collected in regions without reference instrumentation.
Noah Bernays, Daniel A. Jaffe, Irina Petropavlovskikh, and Peter Effertz
Atmos. Meas. Tech., 15, 3189–3192, https://doi.org/10.5194/amt-15-3189-2022, https://doi.org/10.5194/amt-15-3189-2022, 2022
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Ozone is an important pollutant that impacts millions of people worldwide. It is therefore important to ensure accurate measurements. A recent surge in wildfire activity in the USA has resulted in significant enhancements in ozone concentration. However given the nature of wildfire smoke, there are questions about our ability to accurately measure ozone. In this comment, we discuss possible biases in the UV measurements of ozone in the presence of smoke.
Gérard Ancellet, Sophie Godin-Beekmann, Herman G. J. Smit, Ryan M. Stauffer, Roeland Van Malderen, Renaud Bodichon, and Andrea Pazmiño
Atmos. Meas. Tech., 15, 3105–3120, https://doi.org/10.5194/amt-15-3105-2022, https://doi.org/10.5194/amt-15-3105-2022, 2022
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The 1991–2021 Observatoire de Haute Provence electrochemical concentration cell (ECC) ozonesonde data have been homogenized according to the recommendations of the Ozonesonde Data Quality Assessment panel. Comparisons with ground-based instruments also measuring ozone at the same station (lidar, surface measurements) and with colocated satellite observations show the benefits of this homogenization. Remaining differences between ECC and other observations in the stratosphere are also discussed.
Horim Kim, Michael Müller, Stephan Henne, and Christoph Hüglin
Atmos. Meas. Tech., 15, 2979–2992, https://doi.org/10.5194/amt-15-2979-2022, https://doi.org/10.5194/amt-15-2979-2022, 2022
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In this study, the performance of electrochemical sensors for NO and NO2 for measuring air quality was determined over a longer operating period. The performance of NO sensors remained reliable for more than 18 months. However, the NO2 sensors showed decreasing performance over time. During deployment, we found that the NO2 sensors can distinguish general pollution levels, but they proved unsuitable for accurate measurements due to significant biases.
Randulph Morales, Jonas Ravelid, Katarina Vinkovic, Piotr Korbeń, Béla Tuzson, Lukas Emmenegger, Huilin Chen, Martina Schmidt, Sebastian Humbel, and Dominik Brunner
Atmos. Meas. Tech., 15, 2177–2198, https://doi.org/10.5194/amt-15-2177-2022, https://doi.org/10.5194/amt-15-2177-2022, 2022
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Mapping trace gas emission plumes using in situ measurements from unmanned aerial vehicles (UAVs) is an emerging and attractive possibility to quantify emissions from localized sources. We performed an extensive controlled-release experiment to develop an optimal quantification method and to determine the related uncertainties under various environmental and sampling conditions. Our approach was successful in quantifying local methane sources from drone-based measurements.
Junlei Zhan, Yongchun Liu, Wei Ma, Xin Zhang, Xuezhong Wang, Fang Bi, Yujie Zhang, Zhenhai Wu, and Hong Li
Atmos. Meas. Tech., 15, 1511–1520, https://doi.org/10.5194/amt-15-1511-2022, https://doi.org/10.5194/amt-15-1511-2022, 2022
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Our study investigated the O3 formation sensitivity in Beijing using a random forest model coupled with the reactivity of volatile organic
compound (VOC) species. Results found that random forest accurately predicted O3 concentration when initial VOCs were considered, and relative importance correlated well with O3 formation potential. The O3 isopleth curves calculated by the random forest model were generally comparable with those calculated by the box model.
Daniel R. Peters, Olalekan A. M. Popoola, Roderic L. Jones, Nicholas A. Martin, Jim Mills, Elizabeth R. Fonseca, Amy Stidworthy, Ella Forsyth, David Carruthers, Megan Dupuy-Todd, Felicia Douglas, Katie Moore, Rishabh U. Shah, Lauren E. Padilla, and Ramón A. Alvarez
Atmos. Meas. Tech., 15, 321–334, https://doi.org/10.5194/amt-15-321-2022, https://doi.org/10.5194/amt-15-321-2022, 2022
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We present more than 2 years of NO2 pollution measurements from a sensor network in Greater London and compare results to an extensive network of expensive reference-grade monitors. We show the ability of our lower-cost network to generate robust insights about local air pollution. We also show how irregularities in sensor performance lead to some uncertainty in results and demonstrate ways that future users can characterize and mitigate uncertainties to get the most value from sensor data.
Timothy G. Pernini, T. Scott Zaccheo, Jeremy Dobler, and Nathan Blume
Atmos. Meas. Tech., 15, 225–240, https://doi.org/10.5194/amt-15-225-2022, https://doi.org/10.5194/amt-15-225-2022, 2022
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We demonstrate a novel approach to estimating emissions from oil sands operations that utilizes the GreenLITE™ gas concentration measurement system and an atmospheric model. While deployed at a facility in the Athabasca region of Alberta, Canada, CH4 emissions from a tailings pond were estimated to be 7.2 t/d for July–October 2019, and 5.1 t/d for March–July 2020. CH4 emissions from an open-pit mine were estimated to be 24.6 t/d for September–October 2019.
Wengang Zhang, Ling Wang, Yang Yu, Guirong Xu, Xiuqing Hu, Zhikang Fu, and Chunguang Cui
Atmos. Meas. Tech., 14, 7821–7834, https://doi.org/10.5194/amt-14-7821-2021, https://doi.org/10.5194/amt-14-7821-2021, 2021
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Global precipitable water vapor (PWV) derived from MERSI-II (Medium Resolution Spectral Imager) is compared with PWV from the Integrated Global Radiosonde Archive (IGRA). Our results show a good agreement between PWV from MERSI-II and IGRA and that MERSI-II PWV is slightly underestimated on the whole, especially in summer. The bias between MERSI-II and IGRA grows with a larger spatial distance between the footprint of the satellite and the IGRA station, as well as increasing PWV.
Trevor W. Coates, Monzurul Alam, Thomas K. Flesch, and Guillermo Hernandez-Ramirez
Atmos. Meas. Tech., 14, 7147–7152, https://doi.org/10.5194/amt-14-7147-2021, https://doi.org/10.5194/amt-14-7147-2021, 2021
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A field study tested two footprint models for calculating surface emissions from downwind flux measurements. Emission rates from a 10 × 10 m synthetic source were estimated with the simple Kormann–Meixner model and a sophisticated Lagrangian stochastic model. Both models underestimated emissions by approximately 30 %, and no statistical differences were observed between the models. Footprint models are critically important for interpreting eddy covariance measurements.
Teles C. Furlani, Patrick R. Veres, Kathryn E. R. Dawe, J. Andrew Neuman, Steven S. Brown, Trevor C. VandenBoer, and Cora J. Young
Atmos. Meas. Tech., 14, 5859–5871, https://doi.org/10.5194/amt-14-5859-2021, https://doi.org/10.5194/amt-14-5859-2021, 2021
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This study characterized and validated a commercial spectroscopic instrument for the measurement of hydrogen chloride (HCl) in the atmosphere. Near the Earth’s surface, HCl acts as the dominant reservoir for other chlorine-containing reactive chemicals that play an important role in atmospheric chemistry. The properties of HCl make it challenging to measure. This instrument can overcome many of these challenges, enabling reliable HCl measurements.
Attilio Naccarato, Antonella Tassone, Maria Martino, Sacha Moretti, Antonella Macagnano, Emiliano Zampetti, Paolo Papa, Joshua Avossa, Nicola Pirrone, Michelle Nerentorp, John Munthe, Ingvar Wängberg, Geoff W. Stupple, Carl P. J. Mitchell, Adam R. Martin, Alexandra Steffen, Diana Babi, Eric M. Prestbo, Francesca Sprovieri, and Frank Wania
Atmos. Meas. Tech., 14, 3657–3672, https://doi.org/10.5194/amt-14-3657-2021, https://doi.org/10.5194/amt-14-3657-2021, 2021
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Mercury monitoring in support of the Minamata Convention requires effective and reliable analytical tools. Passive sampling is a promising approach for creating a sustainable long-term network for atmospheric mercury with improved spatial resolution and global coverage. In this study the analytical performance of three passive air samplers (CNR-PAS, IVL-PAS, and MerPAS) was assessed over extended deployment periods and the accuracy of concentrations was judged by comparison with active sampling.
Mei Bai, José I. Velazco, Trevor W. Coates, Frances A. Phillips, Thomas K. Flesch, Julian Hill, David G. Mayer, Nigel W. Tomkins, Roger S. Hegarty, and Deli Chen
Atmos. Meas. Tech., 14, 3469–3479, https://doi.org/10.5194/amt-14-3469-2021, https://doi.org/10.5194/amt-14-3469-2021, 2021
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The development and validation of management practices to mitigate methane (CH4) emissions from livestock require accurate emission measurements. We compared the inverse dispersion modelling (IDM) and tracer-ratio techniques to measure CH4 emissions from cattle. Both measurements agreed well but were higher than IPCC estimates. We suggest that the IDM approach can provide an accurate method of estimating cattle emissions, and IPCC estimates may have larger uncertainties.
Yuan You, Ralf M. Staebler, Samar G. Moussa, James Beck, and Richard L. Mittermeier
Atmos. Meas. Tech., 14, 1879–1892, https://doi.org/10.5194/amt-14-1879-2021, https://doi.org/10.5194/amt-14-1879-2021, 2021
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Tailings ponds in the Alberta oil sands can be significant sources of methane, an important greenhouse gas. This paper describes a 1-month study conducted in 2017 to measure methane emissions from a pond using a variety of micrometeorological flux methods and demonstrates some advantages of these methods over flux chambers.
Christoph Häni, Marcel Bühler, Albrecht Neftel, Christof Ammann, and Thomas Kupper
Atmos. Meas. Tech., 14, 1733–1741, https://doi.org/10.5194/amt-14-1733-2021, https://doi.org/10.5194/amt-14-1733-2021, 2021
Seth Kutikoff, Xiaomao Lin, Steven R. Evett, Prasanna Gowda, David Brauer, Jerry Moorhead, Gary Marek, Paul Colaizzi, Robert Aiken, Liukang Xu, and Clenton Owensby
Atmos. Meas. Tech., 14, 1253–1266, https://doi.org/10.5194/amt-14-1253-2021, https://doi.org/10.5194/amt-14-1253-2021, 2021
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Fast-response infrared gas sensors have been used over 3 decades for long-term monitoring of water vapor fluxes. As optically improved infrared gas sensors are newly employed, we evaluated the performance of water vapor density and water vapor flux from three generations of infrared gas sensors in Bushland, Texas, USA. From our experiments, fluxes from the old sensors were best representative of evapotranspiration based on a world-class lysimeter reference measurement.
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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.
Three instruments that use different techniques to measure gaseous formaldehyde concentrations...
