Articles | Volume 22, issue 19
https://doi.org/10.5194/acp-22-13137-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-22-13137-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
12 Oct 2022
Research article |
| 12 Oct 2022
Seasonal variation in nitryl chloride and its relation to gas-phase precursors during the JULIAC campaign in Germany
IEK-8: Troposphere, Institute of Energy and Climate Research, Forschungszentrum Jülich GmbH, Jülich, Germany
Hendrik Fuchs
IEK-8: Troposphere, Institute of Energy and Climate Research, Forschungszentrum Jülich GmbH, Jülich, Germany
Physikalisches Institut, Universität zu Köln, Cologne, Germany
Andreas Hofzumahaus
IEK-8: Troposphere, Institute of Energy and Climate Research, Forschungszentrum Jülich GmbH, Jülich, Germany
William J. Bloss
School of Geography, Earth, and Environmental Sciences, University of Birmingham, Birmingham, UK
Birger Bohn
IEK-8: Troposphere, Institute of Energy and Climate Research, Forschungszentrum Jülich GmbH, Jülich, Germany
Changmin Cho
IEK-8: Troposphere, Institute of Energy and Climate Research, Forschungszentrum Jülich GmbH, Jülich, Germany
Thorsten Hohaus
IEK-8: Troposphere, Institute of Energy and Climate Research, Forschungszentrum Jülich GmbH, Jülich, Germany
Frank Holland
IEK-8: Troposphere, Institute of Energy and Climate Research, Forschungszentrum Jülich GmbH, Jülich, Germany
Chandrakiran Lakshmisha
IEK-8: Troposphere, Institute of Energy and Climate Research, Forschungszentrum Jülich GmbH, Jülich, Germany
IEK-8: Troposphere, Institute of Energy and Climate Research, Forschungszentrum Jülich GmbH, Jülich, Germany
Paul S. Monks
School of Chemistry, University of Leicester, Leicester, UK
Anna Novelli
IEK-8: Troposphere, Institute of Energy and Climate Research, Forschungszentrum Jülich GmbH, Jülich, Germany
Doreen Niether
IEK-8: Troposphere, Institute of Energy and Climate Research, Forschungszentrum Jülich GmbH, Jülich, Germany
Franz Rohrer
IEK-8: Troposphere, Institute of Energy and Climate Research, Forschungszentrum Jülich GmbH, Jülich, Germany
Ralf Tillmann
IEK-8: Troposphere, Institute of Energy and Climate Research, Forschungszentrum Jülich GmbH, Jülich, Germany
Thalassa S. E. Valkenburg
School of Chemistry, University of Leicester, Leicester, UK
Vaishali Vardhan
IEK-8: Troposphere, Institute of Energy and Climate Research, Forschungszentrum Jülich GmbH, Jülich, Germany
now at: Department of Chemistry, University College Cork, Cork, Ireland
Astrid Kiendler-Scharr
IEK-8: Troposphere, Institute of Energy and Climate Research, Forschungszentrum Jülich GmbH, Jülich, Germany
Physikalisches Institut, Universität zu Köln, Cologne, Germany
Andreas Wahner
IEK-8: Troposphere, Institute of Energy and Climate Research, Forschungszentrum Jülich GmbH, Jülich, Germany
School of Chemistry, University of Leicester, Leicester, UK
School of Geography, Earth, and Environmental Sciences, University of Birmingham, Birmingham, UK
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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
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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
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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
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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
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Marc von Hobe, Domenico Taraborrelli, Sascha Alber, Birger Bohn, Hans-Peter Dorn, Hendrik Fuchs, Yun Li, Chenxi Qiu, Franz Rohrer, Roberto Sommariva, Fred Stroh, Zhaofeng Tan, Sergej Wedel, and Anna Novelli
Atmos. Chem. Phys., 23, 10609–10623, https://doi.org/10.5194/acp-23-10609-2023, https://doi.org/10.5194/acp-23-10609-2023, 2023
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Rongrong Wu, Sören R. Zorn, Sungah Kang, Astrid Kiendler-Scharr, Andreas Wahner, and Thomas F. Mentel
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This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
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Midhun George, Maria Dolores Andrés Hernández, Vladyslav Nenakhov, Yangzhuoran Liu, John Philip Burrows, Birger Bohn, Eric Förster, Florian Obersteiner, Andreas Zahn, Theresa Harlaß, Helmut Ziereis, Hans Schlager, Benjamin Schreiner, Flora Kluge, Katja Bigge, and Klaus Pfeilsticker
Atmos. Chem. Phys., 23, 7799–7822, https://doi.org/10.5194/acp-23-7799-2023, https://doi.org/10.5194/acp-23-7799-2023, 2023
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Can Ye, Keding Lu, Xuefei Ma, Wanyi Qiu, Shule Li, Xinping Yang, Chaoyang Xue, Tianyu Zhai, Yuhan Liu, Xuan Li, Yang Li, Haichao Wang, Zhaofeng Tan, Xiaorui Chen, Huabin Dong, Limin Zeng, Min Hu, and Yuanhang Zhang
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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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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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Zaneta Hamryszczak, Dirk Dienhart, Bettina Brendel, Roland Rohloff, Daniel Marno, Monica Martinez, Hartwig Harder, Andrea Pozzer, Birger Bohn, Martin Zöger, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 23, 5929–5943, https://doi.org/10.5194/acp-23-5929-2023, https://doi.org/10.5194/acp-23-5929-2023, 2023
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Hydrogen peroxide is a key contributor to the oxidative chemistry of the atmosphere through its link to the most prominent oxidants controlling its self-cleansing capacity, HOx. During the CAFE-Africa campaign, H2O2 was measured over the Atlantic Ocean and western Africa in August/September 2018. The study gives an overview of the distribution of H2O2 in the upper tropical troposphere and investigates the impact of convective processes in the Intertropical Convergence Zone on the budget of H2O2.
Joanna E. Dyson, Lisa K. Whalley, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Stephen D. Worrall, Asan Bacak, Archit Mehra, Thomas J. Bannan, Hugh Coe, Carl J. Percival, Bin Ouyang, C. Nicholas Hewitt, Roderic L. Jones, Leigh R. Crilley, Louisa J. Kramer, W. Joe F. Acton, William J. Bloss, Supattarachai Saksakulkrai, Jingsha Xu, Zongbo Shi, Roy M. Harrison, Simone Kotthaus, Sue Grimmond, Yele Sun, Weiqi Xu, Siyao Yue, Lianfang Wei, Pingqing Fu, Xinming Wang, Stephen R. Arnold, and Dwayne E. Heard
Atmos. Chem. Phys., 23, 5679–5697, https://doi.org/10.5194/acp-23-5679-2023, https://doi.org/10.5194/acp-23-5679-2023, 2023
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Kezia Lange, Andreas Richter, Anja Schönhardt, Andreas C. Meier, Tim Bösch, André Seyler, Kai Krause, Lisa K. Behrens, Folkard Wittrock, Alexis Merlaud, Frederik Tack, Caroline Fayt, Martina M. Friedrich, Ermioni Dimitropoulou, Michel Van Roozendael, Vinod Kumar, Sebastian Donner, Steffen Dörner, Bianca Lauster, Maria Razi, Christian Borger, Katharina Uhlmannsiek, Thomas Wagner, Thomas Ruhtz, Henk Eskes, Birger Bohn, Daniel Santana Diaz, Nader Abuhassan, Dirk Schüttemeyer, and John P. Burrows
Atmos. Meas. Tech., 16, 1357–1389, https://doi.org/10.5194/amt-16-1357-2023, https://doi.org/10.5194/amt-16-1357-2023, 2023
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We present airborne imaging DOAS and ground-based stationary and car DOAS measurements conducted during the S5P-VAL-DE-Ruhr campaign in the Rhine-Ruhr region. The measurements are used to validate spaceborne NO2 data products from the Sentinel-5 Precursor TROPOspheric Monitoring Instrument (TROPOMI). Auxiliary data of the TROPOMI NO2 retrieval, such as spatially higher resolved a priori NO2 vertical profiles, surface reflectivity, and cloud treatment are investigated to evaluate their impact.
Philip T. M. Carlsson, Luc Vereecken, Anna Novelli, François Bernard, Steven S. Brown, Bellamy Brownwood, Changmin Cho, John N. Crowley, Patrick Dewald, Peter M. Edwards, Nils Friedrich, Juliane L. Fry, Mattias Hallquist, Luisa Hantschke, Thorsten Hohaus, Sungah Kang, Jonathan Liebmann, Alfred W. Mayhew, Thomas Mentel, David Reimer, Franz Rohrer, Justin Shenolikar, Ralf Tillmann, Epameinondas Tsiligiannis, Rongrong Wu, Andreas Wahner, Astrid Kiendler-Scharr, and Hendrik Fuchs
Atmos. Chem. Phys., 23, 3147–3180, https://doi.org/10.5194/acp-23-3147-2023, https://doi.org/10.5194/acp-23-3147-2023, 2023
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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.
Chuan-Yao Lin, Wan-Chin Chen, Yi-Yun Chien, Charles C. K. Chou, Chian-Yi Liu, Helmut Ziereis, Hans Schlager, Eric Förster, Florian Obersteiner, Ovid O. Krüger, Bruna A. Holanda, Mira L. Pöhlker, Katharina Kaiser, Johannes Schneider, Birger Bohn, Klaus Pfeilsticker, Benjamin Weyland, Maria Dolores Andrés Hernández, and John P. Burrows
Atmos. Chem. Phys., 23, 2627–2647, https://doi.org/10.5194/acp-23-2627-2023, https://doi.org/10.5194/acp-23-2627-2023, 2023
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During the EMeRGe campaign in Asia, atmospheric pollutants were measured on board the HALO aircraft. The WRF-Chem model was employed to evaluate the biomass burning (BB) plume transported from Indochina and its impact on the downstream areas. The combination of BB aerosol enhancement with cloud water resulted in a reduction in incoming shortwave radiation at the surface in southern China and the East China Sea, which potentially has significant regional climate implications.
Changmin Cho, Hendrik Fuchs, Andreas Hofzumahaus, Frank Holland, William J. Bloss, Birger Bohn, Hans-Peter Dorn, Marvin Glowania, Thorsten Hohaus, Lu Liu, Paul S. Monks, Doreen Niether, Franz Rohrer, Roberto Sommariva, Zhaofeng Tan, Ralf Tillmann, Astrid Kiendler-Scharr, Andreas Wahner, and Anna Novelli
Atmos. Chem. Phys., 23, 2003–2033, https://doi.org/10.5194/acp-23-2003-2023, https://doi.org/10.5194/acp-23-2003-2023, 2023
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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.
Amir H. Souri, Matthew S. Johnson, Glenn M. Wolfe, James H. Crawford, Alan Fried, Armin Wisthaler, William H. Brune, Donald R. Blake, Andrew J. Weinheimer, Tijl Verhoelst, Steven Compernolle, Gaia Pinardi, Corinne Vigouroux, Bavo Langerock, Sungyeon Choi, Lok Lamsal, Lei Zhu, Shuai Sun, Ronald C. Cohen, Kyung-Eun Min, Changmin Cho, Sajeev Philip, Xiong Liu, and Kelly Chance
Atmos. Chem. Phys., 23, 1963–1986, https://doi.org/10.5194/acp-23-1963-2023, https://doi.org/10.5194/acp-23-1963-2023, 2023
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We have rigorously characterized different sources of error in satellite-based HCHO / NO2 tropospheric columns, a widely used metric for diagnosing near-surface ozone sensitivity. Specifically, the errors were categorized/quantified into (i) an inherent chemistry error, (ii) the decoupled relationship between columns and the near-surface concentration, (iii) the spatial representativeness error of ground satellite pixels, and (iv) the satellite retrieval errors.
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).
Birger Bohn and Insa Lohse
Atmos. Meas. Tech., 16, 209–233, https://doi.org/10.5194/amt-16-209-2023, https://doi.org/10.5194/amt-16-209-2023, 2023
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Optical receivers for solar spectral actinic radiation are designed for angle-independent sensitivities within a hemisphere. Remaining imperfections can be compensated for by receiver-specific corrections based on laboratory characterizations and radiative transfer calculations of spectral radiance distributions. The corrections cover a wide range of realistic atmospheric conditions and were applied to ground-based and airborne measurements in a wavelength range 280–660 nm.
Xinping Yang, Keding Lu, Xuefei Ma, Yue Gao, Zhaofeng Tan, Haichao Wang, Xiaorui Chen, Xin Li, Xiaofeng Huang, Lingyan He, Mengxue Tang, Bo Zhu, Shiyi Chen, Huabin Dong, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 22, 12525–12542, https://doi.org/10.5194/acp-22-12525-2022, https://doi.org/10.5194/acp-22-12525-2022, 2022
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We present the OH and HO2 radical observations at the Shenzhen site (Pearl River Delta, China) in the autumn of 2018. The diurnal maxima were 4.5 × 106 cm−3 for OH and 4.2 × 108 cm−3 for HO2 (including an estimated interference of 23 %–28 % from RO2 radicals during the daytime). The OH underestimation was identified again, and it was attributable to the missing OH sources. HO2 heterogeneous uptake, ROx sources and sinks, and the atmospheric oxidation capacity were evaluated as well.
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.
Simon F. Reifenberg, Anna Martin, Matthias Kohl, Sara Bacer, Zaneta Hamryszczak, Ivan Tadic, Lenard Röder, Daniel J. Crowley, Horst Fischer, Katharina Kaiser, Johannes Schneider, Raphael Dörich, John N. Crowley, Laura Tomsche, Andreas Marsing, Christiane Voigt, Andreas Zahn, Christopher Pöhlker, Bruna A. Holanda, Ovid Krüger, Ulrich Pöschl, Mira Pöhlker, Patrick Jöckel, Marcel Dorf, Ulrich Schumann, Jonathan Williams, Birger Bohn, Joachim Curtius, Hardwig Harder, Hans Schlager, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 22, 10901–10917, https://doi.org/10.5194/acp-22-10901-2022, https://doi.org/10.5194/acp-22-10901-2022, 2022
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In this work we use a combination of observational data from an aircraft campaign and model results to investigate the effect of the European lockdown due to COVID-19 in spring 2020. Using model results, we show that the largest relative changes to the atmospheric composition caused by the reduced emissions are located in the upper troposphere around aircraft cruise altitude, while the largest absolute changes are present at the surface.
Woohui Nam, Changmin Cho, Begie Perdigones, Tae Siek Rhee, and Kyung-Eun Min
Atmos. Meas. Tech., 15, 4473–4487, https://doi.org/10.5194/amt-15-4473-2022, https://doi.org/10.5194/amt-15-4473-2022, 2022
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We describe our vibration-resistant instrument for measuring ambient NO3, NO2, and H2O based on cavity-enhanced absorption spectroscopy. By simultaneous retrieval of H2O with the other species using a measured H2O absorption spectrum, direct quantifications among all species are possible without any pre-treatment for H2O. Our instrument achieves the effective light path to ~101.5 km, which allows the sensitive measurements of NO3 and NO2 as 1.41 pptv and 6.92 ppbv (1σ) in 1 s.
Zaneta T. Hamryszczak, Andrea Pozzer, Florian Obersteiner, Birger Bohn, Benedikt Steil, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 22, 9483–9497, https://doi.org/10.5194/acp-22-9483-2022, https://doi.org/10.5194/acp-22-9483-2022, 2022
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Hydrogen peroxide plays a pivotal role in the chemistry of the atmosphere. Together with organic hydroperoxides, it forms a reservoir for peroxy radicals, which are known to be the key contributors to the self-cleaning processes of the atmosphere. Hydroperoxides were measured over Europe during the BLUESKY campaign in May–June 2020. The paper gives an overview of the distribution of the species in the troposphere and investigates the impact of wet scavenging and deposition on the budget of H2O2.
Jacky Yat Sing Pang, Anna Novelli, Martin Kaminski, Ismail-Hakki Acir, Birger Bohn, Philip T. M. Carlsson, Changmin Cho, Hans-Peter Dorn, Andreas Hofzumahaus, Xin Li, Anna Lutz, Sascha Nehr, David Reimer, Franz Rohrer, Ralf Tillmann, Robert Wegener, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 22, 8497–8527, https://doi.org/10.5194/acp-22-8497-2022, https://doi.org/10.5194/acp-22-8497-2022, 2022
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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.
Marios Panagi, Roberto Sommariva, Zoë L. Fleming, Paul S. Monks, Gongda Lu, Eloise A. Marais, James R. Hopkins, Alastair C. Lewis, Qiang Zhang, James D. Lee, Freya A. Squires, Lisa K. Whalley, Eloise J. Slater, Dwayne E. Heard, Robert Woodward-Massey, Chunxiang Ye, and Joshua D. Vande Hey
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-379, https://doi.org/10.5194/acp-2022-379, 2022
Revised manuscript not accepted
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A dispersion model and a box model were combined to investigate the evolution of VOCs in Beijing once they are emitted from anthropogenic sources. It was determined that during the winter time the VOC concentrations in Beijing are driven predominantly by sources within Beijing and by a combination of transport and chemistry during the summer. Furthermore, the results in the paper highlight the need for a season specific policy.
Xuefei Ma, Zhaofeng Tan, Keding Lu, Xinping Yang, Xiaorui Chen, Haichao Wang, Shiyi Chen, Xin Fang, Shule Li, Xin Li, Jingwei Liu, Ying Liu, Shengrong Lou, Wanyi Qiu, Hongli Wang, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 22, 7005–7028, https://doi.org/10.5194/acp-22-7005-2022, https://doi.org/10.5194/acp-22-7005-2022, 2022
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This paper presents the first OH and HO2 radical observations made in the Yangtze River Delta in China, and strong oxidation capacity is discovered based on direct measurements. The impacts of new OH regeneration mechanisms, monoterpene oxidation, and HO2 uptake processes are examined and discussed. The sources and the factors to sustain such strong oxidation are the key to understanding the ozone pollution formed in this area.
M. Dolores Andrés Hernández, Andreas Hilboll, Helmut Ziereis, Eric Förster, Ovid O. Krüger, Katharina Kaiser, Johannes Schneider, Francesca Barnaba, Mihalis Vrekoussis, Jörg Schmidt, Heidi Huntrieser, Anne-Marlene Blechschmidt, Midhun George, Vladyslav Nenakhov, Theresa Harlass, Bruna A. Holanda, Jennifer Wolf, Lisa Eirenschmalz, Marc Krebsbach, Mira L. Pöhlker, Anna B. Kalisz Hedegaard, Linlu Mei, Klaus Pfeilsticker, Yangzhuoran Liu, Ralf Koppmann, Hans Schlager, Birger Bohn, Ulrich Schumann, Andreas Richter, Benjamin Schreiner, Daniel Sauer, Robert Baumann, Mariano Mertens, Patrick Jöckel, Markus Kilian, Greta Stratmann, Christopher Pöhlker, Monica Campanelli, Marco Pandolfi, Michael Sicard, José L. Gómez-Amo, Manuel Pujadas, Katja Bigge, Flora Kluge, Anja Schwarz, Nikos Daskalakis, David Walter, Andreas Zahn, Ulrich Pöschl, Harald Bönisch, Stephan Borrmann, Ulrich Platt, and John P. Burrows
Atmos. Chem. Phys., 22, 5877–5924, https://doi.org/10.5194/acp-22-5877-2022, https://doi.org/10.5194/acp-22-5877-2022, 2022
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EMeRGe provides a unique set of in situ and remote sensing airborne measurements of trace gases and aerosol particles along selected flight routes in the lower troposphere over Europe. The interpretation uses also complementary collocated ground-based and satellite measurements. The collected data help to improve the current understanding of the complex spatial distribution of trace gases and aerosol particles resulting from mixing, transport, and transformation of pollution plumes over Europe.
Ülkü Alver Şahin, Roy M. Harrison, Mohammed S. Alam, David C. S. Beddows, Dimitrios Bousiotis, Zongbo Shi, Leigh R. Crilley, William Bloss, James Brean, Isha Khanna, and Rulan Verma
Atmos. Chem. Phys., 22, 5415–5433, https://doi.org/10.5194/acp-22-5415-2022, https://doi.org/10.5194/acp-22-5415-2022, 2022
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Wide-range particle size spectra have been measured in three seasons in Delhi and are interpreted in terms of sources and processes. Condensational growth is a major feature of the fine fraction, and a coarse fraction contributes substantially – but only in summer.
Robert Woodward-Massey, Roberto Sommariva, Lisa K. Whalley, Danny R. Cryer, Trevor Ingham, William J1 Bloss, Sam Cox, James D. Lee, Chris P. Reed, Leigh R. Crilley, Louisa J. Kramer, Brian J. Bandy, Grant L. Forster, Claire E. Reeves, Paul S. Monks, and Dwayne E. Heard
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-207, https://doi.org/10.5194/acp-2022-207, 2022
Preprint withdrawn
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We measured radicals (OH, HO2, RO2) and OH reactivity at a UK coastal site and compared our observations to the predictions of an MCMv3.3.1 box model. We find variable agreement between measured and modelled radical concentrations and OH reactivity, where the levels of agreement for individual species display strong dependences on NO concentrations. The most substantial disagreement is found for RO2 at high NO (> 1 ppbv), when RO2 levels are underpredicted by a factor of ~10–30.
Robert Woodward-Massey, Roberto Sommariva, Lisa K. Whalley, Danny R. Cryer, Trevor Ingham, William J. Bloss, Stephen M. Ball, James D. Lee, Chris P. Reed, Leigh R. Crilley, Louisa J. Kramer, Brian J. Bandy, Grant L. Forster, Claire E. Reeves, Paul S. Monks, and Dwayne E. Heard
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-213, https://doi.org/10.5194/acp-2022-213, 2022
Revised manuscript under review for ACP
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We performed a radical (OH, HO2, RO2; total ROx) budget analysis on a dataset collected during a field intensive at a UK coastal site. We found significant differences between calculated HO2 and RO2 production and destruction rates, which should be balanced for such highly reactive radicals under steady state conditions. In addition, ozone production rates were calculated from measured radicals and compared to MCMv3.3.1 model predictions.
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.
Dongwook Kim, Changmin Cho, Seokhan Jeong, Soojin Lee, Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Jason C. Schroder, Jose L. Jimenez, Rainer Volkamer, Donald R. Blake, Armin Wisthaler, Alan Fried, Joshua P. DiGangi, Glenn S. Diskin, Sally E. Pusede, Samuel R. Hall, Kirk Ullmann, L. Gregory Huey, David J. Tanner, Jack Dibb, Christoph J. Knote, and Kyung-Eun Min
Atmos. Chem. Phys., 22, 805–821, https://doi.org/10.5194/acp-22-805-2022, https://doi.org/10.5194/acp-22-805-2022, 2022
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CHOCHO was simulated using a 0-D box model constrained by measurements during the KORUS-AQ mission. CHOCHO concentration was high in large cities, aromatics being the most important precursors. Loss path to aerosol was the highest sink, contributing to ~ 20 % of secondary organic aerosol formation. Our work highlights that simple CHOCHO surface uptake approach is valid only for low aerosol conditions and more work is required to understand CHOCHO solubility in high-aerosol conditions.
Clara M. Nussbaumer, John N. Crowley, Jan Schuladen, Jonathan Williams, Sascha Hafermann, Andreas Reiffs, Raoul Axinte, Hartwig Harder, Cheryl Ernest, Anna Novelli, Katrin Sala, Monica Martinez, Chinmay Mallik, Laura Tomsche, Christian Plass-Dülmer, Birger Bohn, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 18413–18432, https://doi.org/10.5194/acp-21-18413-2021, https://doi.org/10.5194/acp-21-18413-2021, 2021
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HCHO is an important atmospheric trace gas influencing the photochemical processes in the Earth’s atmosphere, including the budget of HOx and the abundance of tropospheric O3. This research presents the photochemical calculations of HCHO and O3 based on three field campaigns across Europe. We show that HCHO production via the oxidation of only four volatile organic compound precursors, i.e., CH4, CH3CHO, C5H8 and CH3OH, can balance the observed loss at all sites well.
Leigh R. Crilley, Louisa J. Kramer, Francis D. Pope, Chris Reed, James D. Lee, Lucy J. Carpenter, Lloyd D. J. Hollis, Stephen M. Ball, and William J. Bloss
Atmos. Chem. Phys., 21, 18213–18225, https://doi.org/10.5194/acp-21-18213-2021, https://doi.org/10.5194/acp-21-18213-2021, 2021
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Nitrous acid (HONO) is a key source of atmospheric oxidants. We evaluate if the ocean surface is a source of HONO for the marine boundary layer, using measurements from two contrasting coastal locations. We observed no evidence for a night-time ocean surface source, in contrast to previous work. This points to significant geographical variation in the predominant HONO formation mechanisms in marine environments, reflecting possible variability in the sea-surface microlayer composition.
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.
Clara M. Nussbaumer, Uwe Parchatka, Ivan Tadic, Birger Bohn, Daniel Marno, Monica Martinez, Roland Rohloff, Hartwig Harder, Flora Kluge, Klaus Pfeilsticker, Florian Obersteiner, Martin Zöger, Raphael Doerich, John N. Crowley, Jos Lelieveld, and Horst Fischer
Atmos. Meas. Tech., 14, 6759–6776, https://doi.org/10.5194/amt-14-6759-2021, https://doi.org/10.5194/amt-14-6759-2021, 2021
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NO2 plays a central role in atmospheric photochemical processes and requires accurate measurements. This research presents NO2 data obtained via chemiluminescence using a photolytic converter from airborne studies around Cabo Verde and laboratory investigations. We show the limits and error-proneness of a conventional blue light converter in aircraft measurements affected by humidity and NO levels and suggest the use of an alternative quartz converter for more reliable results.
Beth S. Nelson, Gareth J. Stewart, Will S. Drysdale, Mike J. Newland, Adam R. Vaughan, Rachel E. Dunmore, Pete M. Edwards, Alastair C. Lewis, Jacqueline F. Hamilton, W. Joe Acton, C. Nicholas Hewitt, Leigh R. Crilley, Mohammed S. Alam, Ülkü A. Şahin, David C. S. Beddows, William J. Bloss, Eloise Slater, Lisa K. Whalley, Dwayne E. Heard, James M. Cash, Ben Langford, Eiko Nemitz, Roberto Sommariva, Sam Cox, Shivani, Ranu Gadi, Bhola R. Gurjar, James R. Hopkins, Andrew R. Rickard, and James D. Lee
Atmos. Chem. Phys., 21, 13609–13630, https://doi.org/10.5194/acp-21-13609-2021, https://doi.org/10.5194/acp-21-13609-2021, 2021
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Ozone production at an urban site in Delhi is sensitive to volatile organic compound (VOC) concentrations, particularly those of the aromatic, monoterpene, and alkene VOC classes. The change in ozone production by varying atmospheric pollutants according to their sources, as defined in an emissions inventory, is investigated. The study suggests that reducing road transport emissions alone does not reduce reactive VOCs in the atmosphere enough to perturb an increase in ozone production.
Paul S. Monks, A. R. Ravishankara, Erika von Schneidemesser, and Roberto Sommariva
Atmos. Chem. Phys., 21, 12909–12948, https://doi.org/10.5194/acp-21-12909-2021, https://doi.org/10.5194/acp-21-12909-2021, 2021
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Which published papers have transformed our understanding of the chemical processes in the troposphere and shaped the field of atmospheric chemistry? We explore how these papers have shaped the development of the field of atmospheric chemistry and identify the major landmarks in the field of atmospheric chemistry through the lens of those papers' impact on science, legislation and environmental events.
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.
Marvin Glowania, Franz Rohrer, Hans-Peter Dorn, Andreas Hofzumahaus, Frank Holland, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Meas. Tech., 14, 4239–4253, https://doi.org/10.5194/amt-14-4239-2021, https://doi.org/10.5194/amt-14-4239-2021, 2021
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Three instruments that use different techniques to measure gaseous formaldehyde concentrations were compared in experiments in the atmospheric simulation chamber SAPHIR at Forschungszentrum Jülich. The results demonstrated the need to correct the baseline in measurements by instruments that use the Hantzsch reaction or make use of cavity ring-down spectroscopy. After applying corrections, all three methods gave accurate and precise measurements within their specifications.
Ivan Tadic, Clara M. Nussbaumer, Birger Bohn, Hartwig Harder, Daniel Marno, Monica Martinez, Florian Obersteiner, Uwe Parchatka, Andrea Pozzer, Roland Rohloff, Martin Zöger, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 8195–8211, https://doi.org/10.5194/acp-21-8195-2021, https://doi.org/10.5194/acp-21-8195-2021, 2021
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Although mechanisms of tropospheric ozone (O3) formation are well understood, studies reporting on ozone formation derived from field measurements are challenging and remain sparse in number. We use airborne measurements to quantify nitric oxide (NO) and O3 distributions in the upper troposphere over the Atlantic Ocean and western Africa and compare our measurements to model simulations. Our results show that NO and ozone formation are greatest over the tropical areas of western Africa.
Karn Vohra, Eloise A. Marais, Shannen Suckra, Louisa Kramer, William J. Bloss, Ravi Sahu, Abhishek Gaur, Sachchida N. Tripathi, Martin Van Damme, Lieven Clarisse, and Pierre-F. Coheur
Atmos. Chem. Phys., 21, 6275–6296, https://doi.org/10.5194/acp-21-6275-2021, https://doi.org/10.5194/acp-21-6275-2021, 2021
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We find satellite observations of atmospheric composition generally reproduce variability in surface air pollution, so we use their long record to estimate air quality trends in major UK and Indian cities. Our trend analysis shows that pollutants targeted with air quality policies have not declined in Delhi and Kanpur but have in London and Birmingham, with the exception of a recent and dramatic increase in reactive volatile organics in London. Unregulated ammonia has increased only in Delhi.
Claire E. Reeves, Graham P. Mills, Lisa K. Whalley, W. Joe F. Acton, William J. Bloss, Leigh R. Crilley, Sue Grimmond, Dwayne E. Heard, C. Nicholas Hewitt, James R. Hopkins, Simone Kotthaus, Louisa J. Kramer, Roderic L. Jones, James D. Lee, Yanhui Liu, Bin Ouyang, Eloise Slater, Freya Squires, Xinming Wang, Robert Woodward-Massey, and Chunxiang Ye
Atmos. Chem. Phys., 21, 6315–6330, https://doi.org/10.5194/acp-21-6315-2021, https://doi.org/10.5194/acp-21-6315-2021, 2021
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The impact of isoprene on atmospheric chemistry is dependent on how its oxidation products interact with other pollutants, specifically nitrogen oxides. Such interactions can lead to isoprene nitrates. We made measurements of the concentrations of individual isoprene nitrate isomers in Beijing and used a model to test current understanding of their chemistry. We highlight areas of uncertainty in understanding, in particular the chemistry following oxidation of isoprene by the nitrate radical.
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.
Steven J. Campbell, Kate Wolfer, Battist Utinger, Joe Westwood, Zhi-Hui Zhang, Nicolas Bukowiecki, Sarah S. Steimer, Tuan V. Vu, Jingsha Xu, Nicholas Straw, Steven Thomson, Atallah Elzein, Yele Sun, Di Liu, Linjie Li, Pingqing Fu, Alastair C. Lewis, Roy M. Harrison, William J. Bloss, Miranda Loh, Mark R. Miller, Zongbo Shi, and Markus Kalberer
Atmos. Chem. Phys., 21, 5549–5573, https://doi.org/10.5194/acp-21-5549-2021, https://doi.org/10.5194/acp-21-5549-2021, 2021
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In this study, we quantify PM2.5 oxidative potential (OP), a metric widely suggested as a potential measure of particle toxicity, in Beijing in summer and winter using four acellular assays. We correlate PM2.5 OP with a comprehensive range of atmospheric and particle composition measurements, demonstrating inter-assay differences and seasonal variation of PM2.5 OP. Using multivariate statistical analysis, we highlight specific particle chemical components and sources that influence OP.
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.
Lisa K. Whalley, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Archit Mehra, Stephen D. Worrall, Asan Bacak, Thomas J. Bannan, Hugh Coe, Carl J. Percival, Bin Ouyang, Roderic L. Jones, Leigh R. Crilley, Louisa J. Kramer, William J. Bloss, Tuan Vu, Simone Kotthaus, Sue Grimmond, Yele Sun, Weiqi Xu, Siyao Yue, Lujie Ren, W. Joe F. Acton, C. Nicholas Hewitt, Xinming Wang, Pingqing Fu, and Dwayne E. Heard
Atmos. Chem. Phys., 21, 2125–2147, https://doi.org/10.5194/acp-21-2125-2021, https://doi.org/10.5194/acp-21-2125-2021, 2021
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To understand how emission controls will impact ozone, an understanding of the sources and sinks of OH and the chemical cycling between peroxy radicals is needed. This paper presents measurements of OH, HO2 and total RO2 taken in central Beijing. The radical observations are compared to a detailed chemistry model, which shows that under low NO conditions, there is a missing OH source. Under high NOx conditions, the model under-predicts RO2 and impacts our ability to model ozone.
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.
Eloise J. Slater, Lisa K. Whalley, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Leigh R. Crilley, Louisa Kramer, William Bloss, Tuan Vu, Yele Sun, Weiqi Xu, Siyao Yue, Lujie Ren, W. Joe F. Acton, C. Nicholas Hewitt, Xinming Wang, Pingqing Fu, and Dwayne E. Heard
Atmos. Chem. Phys., 20, 14847–14871, https://doi.org/10.5194/acp-20-14847-2020, https://doi.org/10.5194/acp-20-14847-2020, 2020
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The paper details atmospheric chemistry in a megacity (Beijing), focussing on radicals which mediate the formation of secondary pollutants such as ozone and particles. Highly polluted conditions were experienced, including the highest ever levels of nitric oxide (NO), with simultaneous radical measurements. Radical concentrations were large during "haze" events, demonstrating active photochemistry. Modelling showed that our understanding of the chemistry at high NOx levels is incomplete.
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.
Sarah S. Steimer, Daniel J. Patton, Tuan V. Vu, Marios Panagi, Paul S. Monks, Roy M. Harrison, Zoë L. Fleming, Zongbo Shi, and Markus Kalberer
Atmos. Chem. Phys., 20, 13303–13318, https://doi.org/10.5194/acp-20-13303-2020, https://doi.org/10.5194/acp-20-13303-2020, 2020
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Air pollution is of growing concern due to its negative effect on public health, especially in low- and middle-income countries. This study investigates how the chemical composition of particles in Beijing changes under different measurement conditions (pollution levels, season) to get a better understanding of the sources of this form of air pollution.
Mohammed S. Alam, Leigh R. Crilley, James D. Lee, Louisa J. Kramer, Christian Pfrang, Mónica Vázquez-Moreno, Milagros Ródenas, Amalia Muñoz, and William J. Bloss
Atmos. Meas. Tech., 13, 5977–5991, https://doi.org/10.5194/amt-13-5977-2020, https://doi.org/10.5194/amt-13-5977-2020, 2020
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We report on the interference arising in measurements of nitrogen oxides (NOx) from the presence of a range of alkenes in sampled air when using the most widespread air quality monitoring technique for chemiluminescence detection. Interferences of up to 11 % are reported, depending upon the alkene present and conditions used. Such interferences may be of substantial importance for the interpretation of ambient NOx data, particularly for high volatile organic compound and low NOx environments.
Bettina Hottmann, Sascha Hafermann, Laura Tomsche, Daniel Marno, Monica Martinez, Hartwig Harder, Andrea Pozzer, Marco Neumaier, Andreas Zahn, Birger Bohn, Greta Stratmann, Helmut Ziereis, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 20, 12655–12673, https://doi.org/10.5194/acp-20-12655-2020, https://doi.org/10.5194/acp-20-12655-2020, 2020
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During OMO we observed enhanced mixing ratios of hydroperoxides (ROOH) in the Asian monsoon anticyclone (AMA) relative to the background. The observed mixing ratios are higher than steady-state calculations and EMAC simulations, especially in the AMA, indicating atmospheric transport of ROOH. Uncertainties in the scavenging efficiencies likely cause deviations from EMAC. Longitudinal gradients indicate a pool of ROOH towards the center of the AMA associated with upwind convection over India.
Ruqian Miao, Qi Chen, Yan Zheng, Xi Cheng, Yele Sun, Paul I. Palmer, Manish Shrivastava, Jianping Guo, Qiang Zhang, Yuhan Liu, Zhaofeng Tan, Xuefei Ma, Shiyi Chen, Limin Zeng, Keding Lu, and Yuanhang Zhang
Atmos. Chem. Phys., 20, 12265–12284, https://doi.org/10.5194/acp-20-12265-2020, https://doi.org/10.5194/acp-20-12265-2020, 2020
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In this study we evaluated the model performances for simulating secondary inorganic aerosol (SIA) and organic aerosol (OA) in PM2.5 in China against comprehensive datasets. The potential biases from factors related to meteorology, emission, chemistry, and atmospheric removal are systematically investigated. This study provides a comprehensive understanding of modeling PM2.5, which is important for studies on the effectiveness of emission control strategies.
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.
Louisa J. Kramer, Leigh R. Crilley, Thomas J. Adams, Stephen M. Ball, Francis D. Pope, and William J. Bloss
Atmos. Chem. Phys., 20, 5231–5248, https://doi.org/10.5194/acp-20-5231-2020, https://doi.org/10.5194/acp-20-5231-2020, 2020
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HONO is a large source of OH radicals, which can drive VOC oxidation, leading to the formation of ozone and secondary organic aerosols. Here we investigate primary vehicle emissions of HONO from measurements in a road tunnel in Birmingham, UK. A HONO/NOx emission ratio was detemined and compared to previous studies. Results indicate HONO/NOx has not varied much over the last two decades and technologies aimed at reducing NO2 may have also resulted in a reduction in direct HONO vehicle emissions.
Cristina Ruiz Villena, Jasdeep S. Anand, Roland J. Leigh, Paul S. Monks, Claire E. Parfitt, and Joshua D. Vande Hey
Atmos. Meas. Tech., 13, 1735–1756, https://doi.org/10.5194/amt-13-1735-2020, https://doi.org/10.5194/amt-13-1735-2020, 2020
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We present a new method to derive NO2 concentrations from satellite observations that uses up to 30 times less spectral information than traditional methods. We tested the method using data from existing instruments OMI and TROPOMI and found our results agree with the reference data to 5 % and 11 %, respectively. Our method could allow for simpler instrument designs that can be used in low-cost constellations of small satellites for air quality monitoring at high spatial and temporal resolution.
Roberto Sommariva, Louisa J. Kramer, Leigh R. Crilley, Mohammed S. Alam, and William J. Bloss
Atmos. Meas. Tech., 13, 1655–1670, https://doi.org/10.5194/amt-13-1655-2020, https://doi.org/10.5194/amt-13-1655-2020, 2020
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Ozone is a key atmospheric pollutant formed through chemical processing of natural and anthropogenic emissions and removed by reaction with organic compounds emitted by plants. We describe a new instrument – the
Total Ozone Reactivity Systemor TORS – that measures the total loss of ozone in the troposphere. The objective of the TORS instrument is to provide an estimate of the organic compounds emitted by plants which are not measured and thus to improve our understanding of the ozone budget.
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.
Leigh R. Crilley, Ajit Singh, Louisa J. Kramer, Marvin D. Shaw, Mohammed S. Alam, Joshua S. Apte, William J. Bloss, Lea Hildebrandt Ruiz, Pingqing Fu, Weiqi Fu, Shahzad Gani, Michael Gatari, Evgenia Ilyinskaya, Alastair C. Lewis, David Ng'ang'a, Yele Sun, Rachel C. W. Whitty, Siyao Yue, Stuart Young, and Francis D. Pope
Atmos. Meas. Tech., 13, 1181–1193, https://doi.org/10.5194/amt-13-1181-2020, https://doi.org/10.5194/amt-13-1181-2020, 2020
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There is considerable interest in using low-cost optical particle counters (OPCs) for particle mass measurements; however, there is no agreed upon method with respect to calibration. Here we exploit a number of datasets globally to demonstrate that particle composition and relative humidity are the key factors affecting measured concentrations from a low-cost OPC, and we present a simple correction methodology that corrects for this influence.
Marios Panagi, Zoë L. Fleming, Paul S. Monks, Matthew J. Ashfold, Oliver Wild, Michael Hollaway, Qiang Zhang, Freya A. Squires, and Joshua D. Vande Hey
Atmos. Chem. Phys., 20, 2825–2838, https://doi.org/10.5194/acp-20-2825-2020, https://doi.org/10.5194/acp-20-2825-2020, 2020
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In this paper, using dispersion modelling with emission inventories it was determined that on average 45 % of the total CO pollution that affects Beijing is transported from other areas. About half of the CO comes from beyond the immediate surrounding areas. Finally three classification types of pollution were identified and used to analyse the APHH winter campaign. The results can inform targeted control measures to be implemented in Beijing and the other regions to tackle air quality problems.
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.
Roberto Sommariva, Sam Cox, Chris Martin, Kasia Borońska, Jenny Young, Peter K. Jimack, Michael J. Pilling, Vasileios N. Matthaios, Beth S. Nelson, Mike J. Newland, Marios Panagi, William J. Bloss, Paul S. Monks, and Andrew R. Rickard
Geosci. Model Dev., 13, 169–183, https://doi.org/10.5194/gmd-13-169-2020, https://doi.org/10.5194/gmd-13-169-2020, 2020
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This paper presents the AtChem software, which can be used to build box models for atmospheric chemistry studies. The software is designed to facilitate the use of one of the most important chemical mechanisms used by atmospheric scientists, the Master Chemical Mechanism. AtChem exists in two versions: an on-line application for laboratory studies and educational or outreach activities and an offline version for more complex models and batch simulations. AtChem is open source under MIT License.
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.
Leigh R. Crilley, Louisa J. Kramer, Bin Ouyang, Jun Duan, Wenqian Zhang, Shengrui Tong, Maofa Ge, Ke Tang, Min Qin, Pinhua Xie, Marvin D. Shaw, Alastair C. Lewis, Archit Mehra, Thomas J. Bannan, Stephen D. Worrall, Michael Priestley, Asan Bacak, Hugh Coe, James Allan, Carl J. Percival, Olalekan A. M. Popoola, Roderic L. Jones, and William J. Bloss
Atmos. Meas. Tech., 12, 6449–6463, https://doi.org/10.5194/amt-12-6449-2019, https://doi.org/10.5194/amt-12-6449-2019, 2019
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Nitrous acid (HONO) is key species for understanding tropospheric chemistry, yet accurate and precise measurements are challenging. Here we report an inter–comparison exercise of a number of instruments that measured HONO in a highly polluted location (Beijing). All instruments agreed on the temporal trends yet displayed divergence in absolute concentrations. The cause of this divergence was unclear, but it may in part be due to spatial variability in instrument location.
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
Horst Fischer, Raoul Axinte, Heiko Bozem, John N. Crowley, Cheryl Ernest, Stefan Gilge, Sascha Hafermann, Hartwig Harder, Korbinian Hens, Ruud H. H. Janssen, Rainer Königstedt, Dagmar Kubistin, Chinmay Mallik, Monica Martinez, Anna Novelli, Uwe Parchatka, Christian Plass-Dülmer, Andrea Pozzer, Eric Regelin, Andreas Reiffs, Torsten Schmidt, Jan Schuladen, and Jos Lelieveld
Atmos. Chem. Phys., 19, 11953–11968, https://doi.org/10.5194/acp-19-11953-2019, https://doi.org/10.5194/acp-19-11953-2019, 2019
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We use in situ observations of H2O2 to study the interplay between photochemistry, transport and deposition processes. The data were obtained during five ground-based field campaigns across Europe. A budget calculation indicates that the photochemical production rate was much larger than photochemical loss and that dry deposition is the dominant loss process. To reproduce the change in H2O2 mixing ratios after sunrise, a variable contribution of entrainment from the residual layer is required.
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.
Sanna Saarikoski, Leah R. Williams, Steven R. Spielman, Gregory S. Lewis, Arantzazu Eiguren-Fernandez, Minna Aurela, Susanne V. Hering, Kimmo Teinilä, Philip Croteau, John T. Jayne, Thorsten Hohaus, Douglas R. Worsnop, and Hilkka Timonen
Atmos. Meas. Tech., 12, 3907–3920, https://doi.org/10.5194/amt-12-3907-2019, https://doi.org/10.5194/amt-12-3907-2019, 2019
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An air-to-air ultrafine particle concentrator (Aerosol Dynamics Inc. concentrator; ADIc) has been tailored for the low (~ 0.08 L min−1) inlet flow of aerosol mass spectrometers, and it provides a factor of 8–21 enrichment in the concentration of particles. The ADIc was evaluated in laboratory and field measurements. The results showed that the concentration factor depends primarily on the ratio between the sample flow and the output flow and is independent of particle size above about 10 nm.
José Dias Neto, Stefan Kneifel, Davide Ori, Silke Trömel, Jan Handwerker, Birger Bohn, Normen Hermes, Kai Mühlbauer, Martin Lenefer, and Clemens Simmer
Earth Syst. Sci. Data, 11, 845–863, https://doi.org/10.5194/essd-11-845-2019, https://doi.org/10.5194/essd-11-845-2019, 2019
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This study describes a 2-month dataset of ground-based, vertically pointing triple-frequency cloud radar observations recorded during the winter season 2015/2016 in Jülich, Germany. Intensive quality control has been applied to the unique long-term dataset, which allows the multifrequency signatures of ice and snow particles to be statistically analyzed for the first time. The analysis includes, for example, aggregation and its dependence on cloud temperature, riming, and onset of melting.
Zongbo Shi, Tuan Vu, Simone Kotthaus, Roy M. Harrison, Sue Grimmond, Siyao Yue, Tong Zhu, James Lee, Yiqun Han, Matthias Demuzere, Rachel E. Dunmore, Lujie Ren, Di Liu, Yuanlin Wang, Oliver Wild, James Allan, W. Joe Acton, Janet Barlow, Benjamin Barratt, David Beddows, William J. Bloss, Giulia Calzolai, David Carruthers, David C. Carslaw, Queenie Chan, Lia Chatzidiakou, Yang Chen, Leigh Crilley, Hugh Coe, Tie Dai, Ruth Doherty, Fengkui Duan, Pingqing Fu, Baozhu Ge, Maofa Ge, Daobo Guan, Jacqueline F. Hamilton, Kebin He, Mathew Heal, Dwayne Heard, C. Nicholas Hewitt, Michael Hollaway, Min Hu, Dongsheng Ji, Xujiang Jiang, Rod Jones, Markus Kalberer, Frank J. Kelly, Louisa Kramer, Ben Langford, Chun Lin, Alastair C. Lewis, Jie Li, Weijun Li, Huan Liu, Junfeng Liu, Miranda Loh, Keding Lu, Franco Lucarelli, Graham Mann, Gordon McFiggans, Mark R. Miller, Graham Mills, Paul Monk, Eiko Nemitz, Fionna O'Connor, Bin Ouyang, Paul I. Palmer, Carl Percival, Olalekan Popoola, Claire Reeves, Andrew R. Rickard, Longyi Shao, Guangyu Shi, Dominick Spracklen, David Stevenson, Yele Sun, Zhiwei Sun, Shu Tao, Shengrui Tong, Qingqing Wang, Wenhua Wang, Xinming Wang, Xuejun Wang, Zifang Wang, Lianfang Wei, Lisa Whalley, Xuefang Wu, Zhijun Wu, Pinhua Xie, Fumo Yang, Qiang Zhang, Yanli Zhang, Yuanhang Zhang, and Mei Zheng
Atmos. Chem. Phys., 19, 7519–7546, https://doi.org/10.5194/acp-19-7519-2019, https://doi.org/10.5194/acp-19-7519-2019, 2019
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APHH-Beijing is a collaborative international research programme to study the sources, processes and health effects of air pollution in Beijing. This introduction to the special issue provides an overview of (i) the APHH-Beijing programme, (ii) the measurement and modelling activities performed as part of it and (iii) the air quality and meteorological conditions during joint intensive field campaigns as a core activity within APHH-Beijing.
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.
Zhaofeng Tan, Keding Lu, Meiqing Jiang, Rong Su, Hongli Wang, Shengrong Lou, Qingyan Fu, Chongzhi Zhai, Qinwen Tan, Dingli Yue, Duohong Chen, Zhanshan Wang, Shaodong Xie, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 19, 3493–3513, https://doi.org/10.5194/acp-19-3493-2019, https://doi.org/10.5194/acp-19-3493-2019, 2019
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We evaluated the atmospheric oxidation capacity (AOC) in four Chinese megacities during photochemically polluted seasons. The chemical production of ozone and particle nitrate was diagnosed through a box model, which can be attributed to daytime radical chemistry. Our work highlights that the formation of both ozone and fine particles is largely driven by the atmospheric radical chemistry in China. Consequently, we suggest future pollution mitigation strategies should consider the role of AOC.
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.
Robbie Ramsay, Chiara F. Di Marco, Mathew R. Heal, Marsailidh M. Twigg, Nicholas Cowan, Matthew R. Jones, Sarah R. Leeson, William J. Bloss, Louisa J. Kramer, Leigh Crilley, Matthias Sörgel, Meinrat Andreae, and Eiko Nemitz
Atmos. Chem. Phys., 18, 16953–16978, https://doi.org/10.5194/acp-18-16953-2018, https://doi.org/10.5194/acp-18-16953-2018, 2018
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Understanding the impact of agricultural activities on the atmosphere requires more measurements of inorganic trace gases and associated aerosol counterparts. This research presents 1 month of measurements above agricultural grassland during a period of fertiliser application. It was found that emissions of the important trace gases ammonia and nitrous acid peaked after fertiliser use and that the velocity at which the measured aerosols were deposited was dependent upon their size.
John N. Crowley, Nicolas Pouvesle, Gavin J. Phillips, Raoul Axinte, Horst Fischer, Tuukka Petäjä, Anke Nölscher, Jonathan Williams, Korbinian Hens, Hartwig Harder, Monica Martinez-Harder, Anna Novelli, Dagmar Kubistin, Birger Bohn, and Jos Lelieveld
Atmos. Chem. Phys., 18, 13457–13479, https://doi.org/10.5194/acp-18-13457-2018, https://doi.org/10.5194/acp-18-13457-2018, 2018
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Simultaneous observations of PAA, PAN and H2O2 are used to provide insight into processes influencing the HOx chemistry of the boreal forest, including two biomass-burning-impacted periods. A significant contribution from photolytic HOx sources was included in a box model analysis to align model predictions with measurements. The model predicts high levels of organic peroxy radicals, also at night-time.
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.
Prasad Kasibhatla, Tomás Sherwen, Mathew J. Evans, Lucy J. Carpenter, Chris Reed, Becky Alexander, Qianjie Chen, Melissa P. Sulprizio, James D. Lee, Katie A. Read, William Bloss, Leigh R. Crilley, William C. Keene, Alexander A. P. Pszenny, and Alma Hodzic
Atmos. Chem. Phys., 18, 11185–11203, https://doi.org/10.5194/acp-18-11185-2018, https://doi.org/10.5194/acp-18-11185-2018, 2018
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Recent measurements of NOx and HONO suggest that photolysis of particulate nitrate in sea-salt aerosols is important in terms of marine boundary layer oxidant chemistry. We present the first global-scale assessment of the significance of this new chemical pathway for NOx, O3, and OH in the marine boundary layer. We also present a preliminary assessment of the potential impact of photolysis of particulate nitrate associated with other aerosol types on continental boundary layer chemistry.
Chinmay Mallik, Laura Tomsche, Efstratios Bourtsoukidis, John N. Crowley, Bettina Derstroff, Horst Fischer, Sascha Hafermann, Imke Hüser, Umar Javed, Stephan Keßel, Jos Lelieveld, Monica Martinez, Hannah Meusel, Anna Novelli, Gavin J. Phillips, Andrea Pozzer, Andreas Reiffs, Rolf Sander, Domenico Taraborrelli, Carina Sauvage, Jan Schuladen, Hang Su, Jonathan Williams, and Hartwig Harder
Atmos. Chem. Phys., 18, 10825–10847, https://doi.org/10.5194/acp-18-10825-2018, https://doi.org/10.5194/acp-18-10825-2018, 2018
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OH and HO2 control the transformation of air pollutants and O3 formation. Their implication for air quality over the climatically sensitive Mediterranean region was studied during a field campaign in Cyprus. Production of OH, HO2, and recycled OH was lower in aged marine air masses. Box model simulations of OH and HO2 agreed with measurements except at high terpene concentrations when model RO2 due to terpenes caused large HO2 loss. Autoxidation schemes for RO2 improved the agreement.
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.
Haichao Wang, Keding Lu, Song Guo, Zhijun Wu, Dongjie Shang, Zhaofeng Tan, Yujue Wang, Michael Le Breton, Shengrong Lou, Mingjin Tang, Yusheng Wu, Wenfei Zhu, Jing Zheng, Limin Zeng, Mattias Hallquist, Min Hu, and Yuanhang Zhang
Atmos. Chem. Phys., 18, 9705–9721, https://doi.org/10.5194/acp-18-9705-2018, https://doi.org/10.5194/acp-18-9705-2018, 2018
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N2O5, ClNO2, and particulate nitrate were measured simultaneously in Beijing, China, in 2016. The elevated N2O5 uptake coefficient and ClNO2 yield were determined, which suggest fast N2O5 uptake in Beijing. We highlight that the NO3 oxidation in nocturnal VOC degradation is efficient, with fast formation of organic nitrates. More studies are needed to investigate NO3–N2O5 chemistry and its contribution to secondary organic aerosol formation.
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.
Mike J. Newland, Andrew R. Rickard, Tomás Sherwen, Mathew J. Evans, Luc Vereecken, Amalia Muñoz, Milagros Ródenas, and William J. Bloss
Atmos. Chem. Phys., 18, 6095–6120, https://doi.org/10.5194/acp-18-6095-2018, https://doi.org/10.5194/acp-18-6095-2018, 2018
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Stabilised Criegee intermediates (SCIs) are formed in the reaction of alkenes with ozone, both of which are ubiquitous throughout the troposphere. We determine the fate and global distribution of SCI from monoterpene ozonolysis. One major fate of SCI is reaction with H2O, but for a fraction of SCIs, unimolecular reactions dominate. Concentrations of SCIs are high enough regionally to play a key role in the conversion of sulfur dioxide to aerosol, affecting air quality and climate.
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.
Birger Bohn and Insa Lohse
Atmos. Meas. Tech., 10, 3151–3174, https://doi.org/10.5194/amt-10-3151-2017, https://doi.org/10.5194/amt-10-3151-2017, 2017
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CCD spectroradiometers are widely used for measurements of atmospheric photolysis frequencies. Their fast response makes them suitable for airborne applications despite the well-known stray-light problem. In this work we describe simple and reliable procedures to minimize the stray-light influence on calibrations and field measurements. Comparisons with a reference instrument confirm high accuracies and low detection limits of important photolysis frequencies.
Bettina Derstroff, Imke Hüser, Efstratios Bourtsoukidis, John N. Crowley, Horst Fischer, Sergey Gromov, Hartwig Harder, Ruud H. H. Janssen, Jürgen Kesselmeier, Jos Lelieveld, Chinmay Mallik, Monica Martinez, Anna Novelli, Uwe Parchatka, Gavin J. Phillips, Rolf Sander, Carina Sauvage, Jan Schuladen, Christof Stönner, Laura Tomsche, and Jonathan Williams
Atmos. Chem. Phys., 17, 9547–9566, https://doi.org/10.5194/acp-17-9547-2017, https://doi.org/10.5194/acp-17-9547-2017, 2017
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The aim of the study was to examine aged air masses being transported from the European continent towards Cyprus. Longer-lived oxygenated volatile organic compounds (OVOCs) such as methanol were mainly impacted by long-distance transport and showed higher values in air masses from eastern Europe than in a flow regime from the west. The impact of the transport through the marine boundary layer as well as the influence of the residual layer/free troposphere on OVOCs were studied.
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.
Anna Novelli, Korbinian Hens, Cheryl Tatum Ernest, Monica Martinez, Anke C. Nölscher, Vinayak Sinha, Pauli Paasonen, Tuukka Petäjä, Mikko Sipilä, Thomas Elste, Christian Plass-Dülmer, Gavin J. Phillips, Dagmar Kubistin, Jonathan Williams, Luc Vereecken, Jos Lelieveld, and Hartwig Harder
Atmos. Chem. Phys., 17, 7807–7826, https://doi.org/10.5194/acp-17-7807-2017, https://doi.org/10.5194/acp-17-7807-2017, 2017
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The ambient concentration of stabilised Criegee intermediates (SCIs) was estimated for two
environments using field data. The low concentrations predicted indicate that SCIs are
unlikely to have a large impact on atmospheric chemistry. Concurrent measurements of an OH background signal using the Mainz IPI-LIF-FAGE instrument were found to be consistent with the chemistry of SCIs during the measurement campaigns.
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.
Andreas Macke, Patric Seifert, Holger Baars, Christian Barthlott, Christoph Beekmans, Andreas Behrendt, Birger Bohn, Matthias Brueck, Johannes Bühl, Susanne Crewell, Thomas Damian, Hartwig Deneke, Sebastian Düsing, Andreas Foth, Paolo Di Girolamo, Eva Hammann, Rieke Heinze, Anne Hirsikko, John Kalisch, Norbert Kalthoff, Stefan Kinne, Martin Kohler, Ulrich Löhnert, Bomidi Lakshmi Madhavan, Vera Maurer, Shravan Kumar Muppa, Jan Schween, Ilya Serikov, Holger Siebert, Clemens Simmer, Florian Späth, Sandra Steinke, Katja Träumner, Silke Trömel, Birgit Wehner, Andreas Wieser, Volker Wulfmeyer, and Xinxin Xie
Atmos. Chem. Phys., 17, 4887–4914, https://doi.org/10.5194/acp-17-4887-2017, https://doi.org/10.5194/acp-17-4887-2017, 2017
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This article provides an overview of the instrumental setup and the main results obtained during the two HD(CP)2 Observational Prototype Experiments HOPE-Jülich and HOPE-Melpitz conducted in Germany in April–May and Sept 2013, respectively. Goal of the field experiments was to provide high-resolution observational datasets for both, improving the understaning of boundary layer and cloud processes, as well as for the evaluation of the new ICON model that is run at 156 m horizontal resolution.
Chris Reed, Mathew J. Evans, Leigh R. Crilley, William J. Bloss, Tomás Sherwen, Katie A. Read, James D. Lee, and Lucy J. Carpenter
Atmos. Chem. Phys., 17, 4081–4092, https://doi.org/10.5194/acp-17-4081-2017, https://doi.org/10.5194/acp-17-4081-2017, 2017
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The source of ozone-depleting compounds in the remote troposphere has been thought to be long-range transport of secondary pollutants such as organic nitrates. Processing of organic nitrates to nitric acid and subsequent deposition on surfaces in the atmosphere was thought to remove these nitrates from the ozone–NOx–HOx cycle. We found through observation of NOx in the remote tropical troposphere at the Cape Verde Observatory that surface nitrates can be released back into the atmosphere.
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.
Ajit Singh, William J. Bloss, and Francis D. Pope
Atmos. Chem. Phys., 17, 2085–2101, https://doi.org/10.5194/acp-17-2085-2017, https://doi.org/10.5194/acp-17-2085-2017, 2017
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Reduced visibility can indicate poor air quality. Using long-term visibility measurements, we explore the combined
influence of aerosol particle and gas characteristics, and meteorology on long-term visibility. The measured
data were fitted to a newly developed light-extinction model to generate predictions of historic aerosol and
gas scattering and absorbing properties. This approach allows for estimation of historic aerosol properties where measurements are not available.
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.
Suad S. Al-Kindi, Francis D. Pope, David C. Beddows, William J. Bloss, and Roy M. Harrison
Atmos. Chem. Phys., 16, 15561–15579, https://doi.org/10.5194/acp-16-15561-2016, https://doi.org/10.5194/acp-16-15561-2016, 2016
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Oleic acid is a chemical substance which is emitted from cooking processes and is present as tiny particles in the atmosphere. The oleic acid in the particles reacts chemically with atmospheric ozone, causing substantial changes to the composition of the particles. This paper uses new techniques to explore these chemical reactions and the effect of humidity upon them. The significance of the results for the atmosphere is considered.
Yee Jun Tham, Zhe Wang, Qinyi Li, Hui Yun, Weihao Wang, Xinfeng Wang, Likun Xue, Keding Lu, Nan Ma, Birger Bohn, Xin Li, Simonas Kecorius, Johannes Größ, Min Shao, Alfred Wiedensohler, Yuanhang Zhang, and Tao Wang
Atmos. Chem. Phys., 16, 14959–14977, https://doi.org/10.5194/acp-16-14959-2016, https://doi.org/10.5194/acp-16-14959-2016, 2016
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This work addresses the unclear global significance of chlorine activation processes in the troposphere. The first high-quality measurement data set of ClNO2 in northern China revealed strong ClNO2 production in the residual layers, and demonstrated its significant effects on radical budget and ozone production. Our findings imply the widespread effects of ClNO2 over the polluted regions of northern China, which may increase photochemical and haze pollution.
Hannah Meusel, Uwe Kuhn, Andreas Reiffs, Chinmay Mallik, Hartwig Harder, Monica Martinez, Jan Schuladen, Birger Bohn, Uwe Parchatka, John N. Crowley, Horst Fischer, Laura Tomsche, Anna Novelli, Thorsten Hoffmann, Ruud H. H. Janssen, Oscar Hartogensis, Michael Pikridas, Mihalis Vrekoussis, Efstratios Bourtsoukidis, Bettina Weber, Jos Lelieveld, Jonathan Williams, Ulrich Pöschl, Yafang Cheng, and Hang Su
Atmos. Chem. Phys., 16, 14475–14493, https://doi.org/10.5194/acp-16-14475-2016, https://doi.org/10.5194/acp-16-14475-2016, 2016
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There are many studies which show discrepancies between modeled and measured nitrous acid (HONO, precursor of OH radical) in the troposphere but with no satisfactory explanation. Ideal conditions to study the unknown sources of HONO were found on Cyprus, a remote Mediterranean island. Budget analysis of trace gas measurements indicates a common source of NO and HONO, which is not related to anthropogenic activity and is most likely derived from biologic activity in soils and subsequent emission.
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.
Birger Bohn, Dwayne E. Heard, Nikolaos Mihalopoulos, Christian Plass-Dülmer, Rainer Schmitt, and Lisa K. Whalley
Atmos. Meas. Tech., 9, 3455–3466, https://doi.org/10.5194/amt-9-3455-2016, https://doi.org/10.5194/amt-9-3455-2016, 2016
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Filter radiometers are instruments that quantify the rate of formation of excited oxygen atoms from photolysis of ozone in the atmosphere. The excited oxygen atoms are important for the atmospheric self-cleaning ability. The radiometers were characterised by measurements of their spectral response. Together with field comparisons with a reference instrument, the characterisations improved the performance. That will help to better understand atmospheric photochemistry in future research.
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.
Simon Schallhart, Pekka Rantala, Eiko Nemitz, Ditte Taipale, Ralf Tillmann, Thomas F. Mentel, Benjamin Loubet, Giacomo Gerosa, Angelo Finco, Janne Rinne, and Taina M. Ruuskanen
Atmos. Chem. Phys., 16, 7171–7194, https://doi.org/10.5194/acp-16-7171-2016, https://doi.org/10.5194/acp-16-7171-2016, 2016
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We present ecosystem exchange fluxes from a mixed oak–hornbeam forest in the Po Valley, Italy. Detectable fluxes were observed for 29 compounds, dominated by isoprene, which comprised over 60 % of the upward flux. Methanol seemed to be deposited to dew, as the deposition happened in the early morning. We estimated that up to 30 % of the upward flux of methyl vinyl ketone and methacrolein originated from atmospheric oxidation of isoprene.
W. Joe F. Acton, Simon Schallhart, Ben Langford, Amy Valach, Pekka Rantala, Silvano Fares, Giulia Carriero, Ralf Tillmann, Sam J. Tomlinson, Ulrike Dragosits, Damiano Gianelle, C. Nicholas Hewitt, and Eiko Nemitz
Atmos. Chem. Phys., 16, 7149–7170, https://doi.org/10.5194/acp-16-7149-2016, https://doi.org/10.5194/acp-16-7149-2016, 2016
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Volatile organic compounds (VOCs) represent a large source of reactive carbon in the atmosphere and hence have a significant impact on air quality. It is therefore important that we can accurately quantify their emission. In this paper we use three methods to determine the fluxes of reactive VOCs from a woodland canopy. We show that two different canopy-scale measurement methods give good agreement, whereas estimates based on leaf-level-based emission underestimate isoprene fluxes.
Chris Reed, Charlotte A. Brumby, Leigh R. Crilley, Louisa J. Kramer, William J. Bloss, Paul W. Seakins, James D. Lee, and Lucy J. Carpenter
Atmos. Meas. Tech., 9, 2483–2495, https://doi.org/10.5194/amt-9-2483-2016, https://doi.org/10.5194/amt-9-2483-2016, 2016
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A new method of measuring nitrous acid (HONO), a potent mediator of air quality in the atmosphere as well as an important indoor pollutant, is presented. The new method relies on simple, proven techniques already widely applied to other atmospheric compounds. The technique can be retrofitted to existing analysers at minimal cost, or developed into instruments capable of very fast measurement which allow for more complex analysis of the behaviour of HONO.
Bernadette Rosati, Erik Herrmann, Silvia Bucci, Federico Fierli, Francesco Cairo, Martin Gysel, Ralf Tillmann, Johannes Größ, Gian Paolo Gobbi, Luca Di Liberto, Guido Di Donfrancesco, Alfred Wiedensohler, Ernest Weingartner, Annele Virtanen, Thomas F. Mentel, and Urs Baltensperger
Atmos. Chem. Phys., 16, 4539–4554, https://doi.org/10.5194/acp-16-4539-2016, https://doi.org/10.5194/acp-16-4539-2016, 2016
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We present vertical profiles of aerosol optical properties, which were explored within the planetary boundary layer in a case study in 2012 in the Po Valley region. A comparison of in situ measurements recorded aboard a Zeppelin NT and ground-based remote-sensing data was performed yielding good agreement. Additionally, the role of ambient relative humidity for the aerosol particles' optical properties was investigated.
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 %.
A. W. H. Chan, N. M. Kreisberg, T. Hohaus, P. Campuzano-Jost, Y. Zhao, D. A. Day, L. Kaser, T. Karl, A. Hansel, A. P. Teng, C. R. Ruehl, D. T. Sueper, J. T. Jayne, D. R. Worsnop, J. L. Jimenez, S. V. Hering, and A. H. Goldstein
Atmos. Chem. Phys., 16, 1187–1205, https://doi.org/10.5194/acp-16-1187-2016, https://doi.org/10.5194/acp-16-1187-2016, 2016
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Using a novel instrument, we have made measurements of organic compounds that can exist as a gas or particle in the rural atmosphere. Through hourly measurements, we have identified the sources and atmospheric processes of these compounds, which are important for modeling the climate and health impact of these emissions.
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.
M. J. Newland, A. R. Rickard, L. Vereecken, A. Muñoz, M. Ródenas, and W. J. Bloss
Atmos. Chem. Phys., 15, 9521–9536, https://doi.org/10.5194/acp-15-9521-2015, https://doi.org/10.5194/acp-15-9521-2015, 2015
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Stabilised Criegee intermediates (SCIs) are formed through alkene-ozone reactions, which occur throughout the atmospheric boundary layer. Recent direct laboratory studies have shown that SCI react rapidly with SO2, NO2 and other trace gases, affecting air quality and climate. We present experimental data from the EUPHORE atmospheric simulation chamber, in which we determine the effects of the ozonolysis of isoprene, on the oxidation of SO2 as a function of H2O and dimethyl sulfide concentration.
P. S. Monks, A. T. Archibald, A. Colette, O. Cooper, M. Coyle, R. Derwent, D. Fowler, C. Granier, K. S. Law, G. E. Mills, D. S. Stevenson, O. Tarasova, V. Thouret, E. von Schneidemesser, R. Sommariva, O. Wild, and M. L. Williams
Atmos. Chem. Phys., 15, 8889–8973, https://doi.org/10.5194/acp-15-8889-2015, https://doi.org/10.5194/acp-15-8889-2015, 2015
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Ozone holds a certain fascination in atmospheric science. It is ubiquitous in the atmosphere, central to tropospheric oxidation chemistry, and yet harmful to human and ecosystem health as well as being an important greenhouse gas. It is not emitted into the atmosphere but is a byproduct of the very oxidation chemistry it largely initiates. This review examines current understanding of the processes regulating tropospheric ozone at global to local scales from both measurements and models.
K. P. Wyche, P. S. Monks, K. L. Smallbone, J. F. Hamilton, M. R. Alfarra, A. R. Rickard, G. B. McFiggans, M. E. Jenkin, W. J. Bloss, A. C. Ryan, C. N. Hewitt, and A. R. MacKenzie
Atmos. Chem. Phys., 15, 8077–8100, https://doi.org/10.5194/acp-15-8077-2015, https://doi.org/10.5194/acp-15-8077-2015, 2015
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This paper describes a new ensemble methodology for the statistical analysis of atmospheric gas- & particle-phase composition data sets. The methodology reduces the huge amount of data derived from many chamber experiments to show that organic reactivity & resultant particle formation can be mapped into unique clusters in statistical space. The model generated is used to map more realistic plant mesocosm oxidation data, the projection of which gives insight into reactive pathways & precursors.
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.
L. R. Crilley, W. J. Bloss, J. Yin, D. C. S. Beddows, R. M. Harrison, J. D. Allan, D. E. Young, M. Flynn, P. Williams, P. Zotter, A. S. H. Prevot, M. R. Heal, J. F. Barlow, C. H. Halios, J. D. Lee, S. Szidat, and C. Mohr
Atmos. Chem. Phys., 15, 3149–3171, https://doi.org/10.5194/acp-15-3149-2015, https://doi.org/10.5194/acp-15-3149-2015, 2015
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Wood is a renewable fuel but its combustion for residential heating releases a number of locally acting air pollutants, most notably particulate matter known to have adverse effects on human health. This paper used chemical tracers for wood smoke to estimate the contribution that burning wood makes to concentrations of airborne particles in the atmosphere of southern England and most particularly in London.
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
R. Oswald, M. Ermel, K. Hens, A. Novelli, H. G. Ouwersloot, P. Paasonen, T. Petäjä, M. Sipilä, P. Keronen, J. Bäck, R. Königstedt, Z. Hosaynali Beygi, H. Fischer, B. Bohn, D. Kubistin, H. Harder, M. Martinez, J. Williams, T. Hoffmann, I. Trebs, and M. Sörgel
Atmos. Chem. Phys., 15, 799–813, https://doi.org/10.5194/acp-15-799-2015, https://doi.org/10.5194/acp-15-799-2015, 2015
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Nitrous acid (HONO) is a key species in atmospheric photochemistry since the photolysis leads to the important hydroxyl radical (OH). Although the importance of HONO as a precursor of OH is known, the formation pathways of HONO, especially during daytime, are a major challenge in atmospheric science. We present a detailed analysis of sources and sinks for HONO in the atmosphere for a field measurement campaign in the boreal forest in Finland and wonder if there is really a source term missing.
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.
A. Novelli, K. Hens, C. Tatum Ernest, D. Kubistin, E. Regelin, T. Elste, C. Plass-Dülmer, M. Martinez, J. Lelieveld, and H. Harder
Atmos. Meas. Tech., 7, 3413–3430, https://doi.org/10.5194/amt-7-3413-2014, https://doi.org/10.5194/amt-7-3413-2014, 2014
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
K. Hens, A. Novelli, M. Martinez, J. Auld, R. Axinte, B. Bohn, H. Fischer, P. Keronen, D. Kubistin, A. C. Nölscher, R. Oswald, P. Paasonen, T. Petäjä, E. Regelin, R. Sander, V. Sinha, M. Sipilä, D. Taraborrelli, C. Tatum Ernest, J. Williams, J. Lelieveld, and H. Harder
Atmos. Chem. Phys., 14, 8723–8747, https://doi.org/10.5194/acp-14-8723-2014, https://doi.org/10.5194/acp-14-8723-2014, 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. L. Pereira, J. F. Hamilton, A. R. Rickard, W. J. Bloss, M. S. Alam, M. Camredon, A. Muñoz, M. Vázquez, E. Borrás, and M. Ródenas
Atmos. Chem. Phys., 14, 5349–5368, https://doi.org/10.5194/acp-14-5349-2014, https://doi.org/10.5194/acp-14-5349-2014, 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
C. Fricke, A. Ehrlich, E. Jäkel, B. Bohn, M. Wirth, and M. Wendisch
Atmos. Chem. Phys., 14, 1943–1958, https://doi.org/10.5194/acp-14-1943-2014, https://doi.org/10.5194/acp-14-1943-2014, 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
M. Dall'Osto, X. Querol, A. Alastuey, M. C. Minguillon, M. Alier, F. Amato, M. Brines, M. Cusack, J. O. Grimalt, A. Karanasiou, T. Moreno, M. Pandolfi, J. Pey, C. Reche, A. Ripoll, R. Tauler, B. L. Van Drooge, M. Viana, R. M. Harrison, J. Gietl, D. Beddows, W. Bloss, C. O'Dowd, D. Ceburnis, G. Martucci, N. L. Ng, D. Worsnop, J. Wenger, E. Mc Gillicuddy, J. Sodeau, R. Healy, F. Lucarelli, S. Nava, J. L. Jimenez, F. Gomez Moreno, B. Artinano, A. S. H. Prévôt, L. Pfaffenberger, S. Frey, F. Wilsenack, D. Casabona, P. Jiménez-Guerrero, D. Gross, and N. Cots
Atmos. Chem. Phys., 13, 8991–9019, https://doi.org/10.5194/acp-13-8991-2013, https://doi.org/10.5194/acp-13-8991-2013, 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 | Research Activity: Field Measurements | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
High potential for CH4 emission mitigation from oil infrastructure in one of EU's major production regions
Measurement report: Source apportionment and environmental impacts of volatile organic compounds (VOCs) in Lhasa, a highland city in China
OH, HO2, and RO2 radical chemistry in a rural forest environment: measurements, model comparisons, and evidence of a missing radical sink
The atmospheric fate of 1,2-dibromo-4-(1,2-dibromoethyl)cyclohexane (TBECH): spatial patterns, seasonal variability, and deposition to Canadian coastal regions
A single-point modeling approach for the intercomparison and evaluation of ozone dry deposition across chemical transport models (Activity 2 of AQMEII4)
Direct observations of NOx emissions over the San Joaquin Valley using airborne flux measurements during RECAP-CA 2021 field campaign
Trends and seasonal variability in ammonia across major biomes in western and central Africa inferred from long-term series of ground-based and satellite measurements
A rise in HFC-23 emissions from eastern Asia since 2015
Measurement report: Inland ship emissions and their contribution to NOx and ultrafine particle concentrations at the Rhine
Variation and trend of nitrate radical reactivity towards volatile organic compounds in Beijing, China
Intra- and interannual changes in isoprene emission from central Amazonia
Levels of persistent organic pollutants (POPs) in the Antarctic atmosphere over time (1980 to 2021) and estimation of their atmospheric half-lives
Airborne observations of peroxy radicals during the EMeRGe campaign in Europe
Vertical distribution of sources and sinks of volatile organic compounds within a boreal forest canopy
O3 and PAN in southern Tibetan Plateau determined by distinct physical and chemical processes
Technical note: Isolating methane emissions from animal feeding operations in an interfering location
Exploring the amplied role of HCHO during the wintertime ozone and PM2.5 pollution in a coastal city of southeast China
Measurement report: Atmospheric CH4 at regional stations of the Korea Meteorological Administration–Global Atmosphere Watch Programme: measurement, characteristics, and long-term changes of its drivers
Measurement report: MAX-DOAS measurements characterise Central London ozone pollution episodes during 2022 heatwaves
OH measurements in the coastal atmosphere of South China: possible missing OH sinks in aged air masses
Measurement report: Underestimated reactive organic gases from residential combustion – insights from a near-complete speciation
Quantification of fossil fuel CO2 from combined CO, δ13CO2 and Δ14CO2 observations
Measurement report: Hydrogen peroxide in the upper tropical troposphere over the Atlantic Ocean and western Africa during the CAFE-Africa aircraft campaign
A new insight into the vertical differences in NO2 heterogeneous reaction to produce HONO over inland and marginal seas
Chemical identification of new particle formation and growth precursors through positive matrix factorization of ambient ion measurements
Snowpack nitrate photolysis drives the summertime atmospheric nitrous acid (HONO) budget in coastal Antarctica
Revealing the sources and sinks of negative cluster ions in an urban environment through quantitative analysis
Influence of anthropogenic emissions on the composition of highly oxygenated organic molecules in Helsinki: a street canyon and urban background station comparison
Volatile organic compound fluxes in the San Joaquin Valley – spatial distribution, source attribution, and inventory comparison
Measurement report: Molecular-level investigation of atmospheric cluster ions at the tropical high-altitude research station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes
First Measurements of the Nitrogen Stable Isotope Composition (δ15N) of Ship-emitted NOx
Measurement report: Airborne measurements of NOx fluxes over Los Angeles during the RECAP-CA 2021 campaign
Observations of biogenic volatile organic compounds over a mixed temperate forest during the summer to autumn transition
Unexpectedly high concentrations of atmospheric mercury species in Lhasa, the largest city in the Tibetan Plateau
Real-time measurements of non-methane volatile organic compounds in the central Indo-Gangetic basin, Lucknow, India: source characterisation and their role in O3 and secondary organic aerosol formation
Measurement report: Production and loss of atmospheric formaldehyde at a suburban site of Shanghai in summertime
Measurement report: Volatile organic compound characteristics of the different land-use types in Shanghai: spatiotemporal variation, source apportionment and impact on secondary formations of ozone and aerosol
O3–precursor relationship over multiple patterns of timescale: a case study in Zibo, Shandong Province, China
High emission rates and strong temperature response make boreal wetlands a large source of isoprene and terpenes
Elucidate the formation mechanism of particulate nitrate based on direct radical observations in the Yangtze River Delta summer 2019
Pandemic restrictions in 2020 highlight the significance of non-road NOx sources in central London
Measurement report: Emission factors of NH3 and NHx for wildfires and agricultural fires in the United States
Experimental chemical budgets of OH, HO2, and RO2 radicals in rural air in western Germany during the JULIAC campaign 2019
Chemical and dynamical identification of emission outflows during the HALO campaign EMeRGe in Europe and Asia
Flaring efficiencies and NOx emission ratios measured for offshore oil and gas facilities in the North Sea
Measurement report: Long-range transport and the fate of dimethyl sulfide oxidation products in the free troposphere derived from observations at the high-altitude research station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes
Aircraft-based mass balance estimate of methane emissions from offshore gas facilities in the Southern North Sea
Formaldehyde and hydroperoxide distribution around the Arabian Peninsula – evaluation of EMAC model results with ship-based measurements
Heterogeneity and chemical reactivity of the remote troposphere defined by aircraft measurements – corrected
Fundamental oxidation processes in the remote marine atmosphere investigated using the NO–NO2–O3 photostationary state
Foteini Stavropoulou, Katarina Vinković, Bert Kers, Marcel de Vries, Steven van Heuven, Piotr Korbeń, Martina Schmidt, Julia Wietzel, Pawel Jagoda, Jaroslav M. Necki, Jakub Bartyzel, Hossein Maazallahi, Malika Menoud, Carina van der Veen, Sylvia Walter, Béla Tuzson, Jonas Ravelid, Randulph Paulo Morales, Lukas Emmenegger, Dominik Brunner, Michael Steiner, Arjan Hensen, Ilona Velzeboer, Pim van den Bulk, Hugo Denier van der Gon, Antonio Delre, Maklawe Essonanawe Edjabou, Charlotte Scheutz, Marius Corbu, Sebastian Iancu, Denisa Moaca, Alin Scarlat, Alexandru Tudor, Ioana Vizireanu, Andreea Calcan, Magdalena Ardelean, Sorin Ghemulet, Alexandru Pana, Aurel Constantinescu, Lucian Cusa, Alexandru Nica, Calin Baciu, Cristian Pop, Andrei Radovici, Alexandru Mereuta, Horatiu Stefanie, Alexandru Dandocsi, Bas Hermans, Stefan Schwietzke, Daniel Zavala-Araiza, Huilin Chen, and Thomas Röckmann
Atmos. Chem. Phys., 23, 10399–10412, https://doi.org/10.5194/acp-23-10399-2023, https://doi.org/10.5194/acp-23-10399-2023, 2023
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In this study, we quantify CH4 emissions from onshore oil production sites in Romania at source and facility level using a combination of ground- and drone-based measurement techniques. We show that the total CH4 emissions in our studied areas are much higher than the emissions reported to UNFCCC, and up to three-quarters of the detected emissions are related to operational venting. Our results suggest that oil and gas production infrastructure in Romania holds a massive mitigation potential.
Chunxiang Ye, Shuzheng Guo, Weili Lin, Fangjie Tian, Jianshu Wang, Chong Zhang, Suzhen Chi, Yi Chen, Yingjie Zhang, Limin Zeng, Xin Li, Duo Bu, Jiacheng Zhou, and Weixiong Zhao
Atmos. Chem. Phys., 23, 10383–10397, https://doi.org/10.5194/acp-23-10383-2023, https://doi.org/10.5194/acp-23-10383-2023, 2023
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Online volatile organic compound (VOC) measurements by gas chromatography–mass spectrometry, with other O3 precursors, were used to identify key VOC and other key sources in Lhasa. Total VOCs (TVOCs), alkanes, and aromatics are half as abundant as in Beijing. Oxygenated VOCs (OVOCs) consist of 52 % of the TVOCs. Alkenes and OVOCs account for 80 % of the ozone formation potential. Aromatics dominate secondary organic aerosol potential. Positive matrix factorization decomposed residential sources.
Brandon Bottorff, Michelle M. Lew, Youngjun Woo, Pamela Rickly, Matthew D. Rollings, Benjamin Deming, Daniel C. Anderson, Ezra Wood, Hariprasad D. Alwe, Dylan B. Millet, Andrew Weinheimer, Geoff Tyndall, John Ortega, Sebastien Dusanter, Thierry Leonardis, James Flynn, Matt Erickson, Sergio Alvarez, Jean C. Rivera-Rios, Joshua D. Shutter, Frank Keutsch, Detlev Helmig, Wei Wang, Hannah M. Allen, Johnathan H. Slade, Paul B. Shepson, Steven Bertman, and Philip S. Stevens
Atmos. Chem. Phys., 23, 10287–10311, https://doi.org/10.5194/acp-23-10287-2023, https://doi.org/10.5194/acp-23-10287-2023, 2023
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The hydroxyl (OH), hydroperoxy (HO2), and organic peroxy (RO2) radicals play important roles in atmospheric chemistry and have significant air quality implications. Here, we compare measurements of OH, HO2, and total peroxy radicals (XO2) made in a remote forest in Michigan, USA, to predictions from a series of chemical models. Lower measured radical concentrations suggest that the models may be missing an important radical sink and overestimating the rate of ozone production in this forest.
Jenny Oh, Chubashini Shunthirasingham, Ying Duan Lei, Faqiang Zhan, Yuening Li, Abigaëlle Dalpé Castilloux, Amina Ben Chaaben, Zhe Lu, Kelsey Lee, Frank A. P. C. Gobas, Sabine Eckhardt, Nick Alexandrou, Hayley Hung, and Frank Wania
Atmos. Chem. Phys., 23, 10191–10205, https://doi.org/10.5194/acp-23-10191-2023, https://doi.org/10.5194/acp-23-10191-2023, 2023
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An emerging brominated flame retardant (BFR) called TBECH (1,2-dibromo-4-(1,2-dibromoethyl)cyclohexane) has never been produced or imported for use in Canada yet is found to be one of the most abundant gaseous BFRs in the Canadian atmosphere. The recorded spatial and temporal variability of TBECH suggest that the release from imported consumer products containing TBECH is the most likely explanation for its environmental occurrence in Canada.
Olivia E. Clifton, Donna Schwede, Christian Hogrefe, Jesse O. Bash, Sam Bland, Philip Cheung, Mhairi Coyle, Lisa Emberson, Johannes Flemming, Erick Fredj, Stefano Galmarini, Laurens Ganzeveld, Orestis Gazetas, Ignacio Goded, Christopher D. Holmes, László Horváth, Vincent Huijnen, Qian Li, Paul A. Makar, Ivan Mammarella, Giovanni Manca, J. William Munger, Juan L. Pérez-Camanyo, Jonathan Pleim, Limei Ran, Roberto San Jose, Sam J. Silva, Ralf Staebler, Shihan Sun, Amos P. K. Tai, Eran Tas, Timo Vesala, Tamás Weidinger, Zhiyong Wu, and Leiming Zhang
Atmos. Chem. Phys., 23, 9911–9961, https://doi.org/10.5194/acp-23-9911-2023, https://doi.org/10.5194/acp-23-9911-2023, 2023
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A primary sink of air pollutants is dry deposition. Dry deposition estimates differ across the models used to simulate atmospheric chemistry. Here, we introduce an effort to examine dry deposition schemes from atmospheric chemistry models. We provide our approach’s rationale, document the schemes, and describe datasets used to drive and evaluate the schemes. We also launch the analysis of results by evaluating against observations and identifying the processes leading to model–model differences.
Qindan Zhu, Bryan Place, Eva Y. Pfannerstill, Sha Tong, Huanxin Zhang, Jun Wang, Clara M. Nussbaumer, Paul Wooldridge, Benjamin C. Schulze, Caleb Arata, Anthony Bucholtz, John H. Seinfeld, Allen H. Goldstein, and Ronald C. Cohen
Atmos. Chem. Phys., 23, 9669–9683, https://doi.org/10.5194/acp-23-9669-2023, https://doi.org/10.5194/acp-23-9669-2023, 2023
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Nitrogen oxide (NOx) is a hazardous air pollutant, and it is the precursor of short-lived climate forcers like tropospheric ozone and aerosol particles. While NOx emissions from transportation has been strictly regulated, soil NOx emissions are overlooked. We use the airborne flux measurements to observe NOx emissions from highways and urban and cultivated soil land cover types. We show non-negligible soil NOx emissions, which are significantly underestimated in current model simulations.
Money Ossohou, Jonathan Edward Hickman, Lieven Clarisse, Pierre-François Coheur, Martin Van Damme, Marcellin Adon, Véronique Yoboué, Eric Gardrat, Maria Dias Alvès, and Corinne Galy-Lacaux
Atmos. Chem. Phys., 23, 9473–9494, https://doi.org/10.5194/acp-23-9473-2023, https://doi.org/10.5194/acp-23-9473-2023, 2023
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The updated analyses of ground-based concentrations and satellite total vertical columns of atmospheric ammonia help us to better understand 21st century ammonia dynamics in sub-Saharan Africa. We conclude that the drivers of trends are agriculture in the dry savanna of Katibougou, Mali; air temperature and agriculture in the wet savanna of Djougou, Benin, and Lamto, Côte d'Ivoire; and leaf area index, air temperature, residential, and agriculture in forests of Bomassa, Republic of Congo.
Hyeri Park, Jooil Kim, Haklim Choi, Sohyeon Geum, Yeaseul Kim, Rona L. Thompson, Jens Mühle, Peter K. Salameh, Christina M. Harth, Kieran M. Stanley, Simon O'Doherty, Paul J. Fraser, Peter G. Simmonds, Paul B. Krummel, Ray F. Weiss, Ronald G. Prinn, and Sunyoung Park
Atmos. Chem. Phys., 23, 9401–9411, https://doi.org/10.5194/acp-23-9401-2023, https://doi.org/10.5194/acp-23-9401-2023, 2023
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Based on atmospheric HFC-23 observations, the first estimate of post-CDM HFC-23 emissions in eastern Asia for 2008–2019 shows that these emissions contribute significantly to the global emissions rise. The observation-derived emissions were much larger than the bottom-up estimates expected to approach zero after 2015 due to national abatement activities. These discrepancies could be attributed to unsuccessful factory-level HFC-23 abatement and inaccurate quantification of emission reductions.
Philipp Eger, Theresa Mathes, Alex Zavarsky, and Lars Duester
Atmos. Chem. Phys., 23, 8769–8788, https://doi.org/10.5194/acp-23-8769-2023, https://doi.org/10.5194/acp-23-8769-2023, 2023
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We investigated the contribution of inland shipping to air pollution at the river Rhine in Germany. Land-based measurements of gaseous and particulate pollutants were carried out for more than 1 year to provide a realistic estimate for the exposure of people to air pollution close to the riverside. Emissions of nitrogen oxides and particulate matter relative to the amount of fuel used, as well as their dependence on ship size, engine type and operating conditions, were examined.
Hejun Hu, Haichao Wang, Keding Lu, Jie Wang, Zelong Zheng, Xuezhen Xu, Tianyu Zhai, Xiaorui Chen, Xiao Lu, Wenxing Fu, Xin Li, Limin Zeng, Min Hu, Yuanhang Zhang, and Shaojia Fan
Atmos. Chem. Phys., 23, 8211–8223, https://doi.org/10.5194/acp-23-8211-2023, https://doi.org/10.5194/acp-23-8211-2023, 2023
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Nitrate radical chemistry is critical to the degradation of volatile organic compounds (VOCs) and secondary organic aerosol formation. This work investigated the level, seasonal variation, and trend of nitrate radical reactivity towards volatile organic compounds (kNO3) in Beijing. We show the key role of isoprene and styrene in regulating seasonal variation in kNO3 and rebuild a long-term record of kNO3 based on the reported VOC measurements.
Eliane Gomes Alves, Raoni Aquino Santana, Cléo Quaresma Dias-Júnior, Santiago Botía, Tyeen Taylor, Ana Maria Yáñez-Serrano, Jürgen Kesselmeier, Efstratios Bourtsoukidis, Jonathan Williams, Pedro Ivo Lembo Silveira de Assis, Giordane Martins, Rodrigo de Souza, Sérgio Duvoisin Júnior, Alex Guenther, Dasa Gu, Anywhere Tsokankunku, Matthias Sörgel, Bruce Nelson, Davieliton Pinto, Shujiro Komiya, Diogo Martins Rosa, Bettina Weber, Cybelli Barbosa, Michelle Robin, Kenneth J. Feeley, Alvaro Duque, Viviana Londoño Lemos, Maria Paula Contreras, Alvaro Idarraga, Norberto López, Chad Husby, Brett Jestrow, and Iván Mauricio Cely Toro
Atmos. Chem. Phys., 23, 8149–8168, https://doi.org/10.5194/acp-23-8149-2023, https://doi.org/10.5194/acp-23-8149-2023, 2023
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Isoprene is emitted mainly by plants and can influence atmospheric chemistry and air quality. But, there are uncertainties in model emission estimates and follow-up atmospheric processes. In our study, with long-term observational datasets of isoprene and biological and environmental factors from central Amazonia, we show that isoprene emission estimates could be improved when biological processes were mechanistically incorporated into the model.
Thais Luarte, Victoria A. Gómez-Aburto, Ignacio Poblete-Castro, Eduardo Castro-Nallar, Nicolas Huneeus, Marco Molina-Montenegro, Claudia Egas, Germán Azcune, Andrés Pérez-Parada, Rainier Lohmann, Pernilla Bohlin-Nizzetto, Jordi Dachs, Susan Bengtson-Nash, Gustavo Chiang, Karla Pozo, and Cristóbal J. Galbán-Malagón
Atmos. Chem. Phys., 23, 8103–8118, https://doi.org/10.5194/acp-23-8103-2023, https://doi.org/10.5194/acp-23-8103-2023, 2023
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In the last 40 years, different research groups have reported on the atmospheric concentrations of persistent organic pollutants in Antarctica. In the present work, we make a compilation to understand the historical trends and estimate the atmospheric half-life of each compound. Of the compounds studied, HCB was the only one that showed no clear trend, while the rest of the studied compounds showed a significant decrease over time. This is consistent with results for polar and sub-polar zones.
Midhun George, Maria Dolores Andrés Hernández, Vladyslav Nenakhov, Yangzhuoran Liu, John Philip Burrows, Birger Bohn, Eric Förster, Florian Obersteiner, Andreas Zahn, Theresa Harlaß, Helmut Ziereis, Hans Schlager, Benjamin Schreiner, Flora Kluge, Katja Bigge, and Klaus Pfeilsticker
Atmos. Chem. Phys., 23, 7799–7822, https://doi.org/10.5194/acp-23-7799-2023, https://doi.org/10.5194/acp-23-7799-2023, 2023
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The applicability of photostationary steady-state (PSS) assumptions to estimate the amount of the sum of peroxy radicals (RO2*) during the EMeRGe airborne observations from the known radical chemistry and onboard measurements of RO2* precursors, photolysis frequencies, and other trace gases such as NOx and O3 was investigated. The comparison of the calculated RO2* with the actual measurements provides an insight into the main processes controlling their concentration in the air masses measured.
Ross Petersen, Thomas Holst, Meelis Mölder, Natascha Kljun, and Janne Rinne
Atmos. Chem. Phys., 23, 7839–7858, https://doi.org/10.5194/acp-23-7839-2023, https://doi.org/10.5194/acp-23-7839-2023, 2023
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We investigate variability in the vertical distribution of volatile organic compounds (VOCs) in boreal forest, determined through multiyear measurements at several heights in a boreal forest in Sweden. VOC source/sink seasonality in canopy was explored using these vertical profiles and with measurements from a collection of sonic anemometers on the station flux tower. Our results show seasonality in the source/sink distribution for several VOCs, such as monoterpenes and water-soluble compounds.
Wanyun Xu, Yuxuan Bian, Weili Lin, Yingjie Zhang, Yaru Wang, Zhiqiang Ma, Xiaoyi Zhang, Gen Zhang, Chunxiang Ye, and Xiaobin Xu
Atmos. Chem. Phys., 23, 7635–7652, https://doi.org/10.5194/acp-23-7635-2023, https://doi.org/10.5194/acp-23-7635-2023, 2023
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Tropospheric ozone (O3) and peroxyacetyl nitrate (PAN) are both photochemical pollutants harmful to the ecological environment and human health, especially in the Tibetan Plateau (TP). However, the factors determining their variations in the TP have not been comprehensively investigated. Results from field measurements and observation-based models revealed that day-to-day variations in O3 and PAN were in fact controlled by distinct physiochemical processes.
Megan E. McCabe, Ilana B. Pollack, Emily V. Fischer, Kathryn M. Steinmann, and Dana R. Caulton
Atmos. Chem. Phys., 23, 7479–7494, https://doi.org/10.5194/acp-23-7479-2023, https://doi.org/10.5194/acp-23-7479-2023, 2023
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Agriculture emissions, including those from beef and dairy cattle feeding operations, make up a large portion of the United States’ total greenhouse gas emissions, but many of these operations reside in areas where methane from oil and natural gas is prevalent, making it difficult to attribute methane in these areas. This work investigates two approaches to emission attribution for cattle feeding operations and provides guidance for emission attribution in other complicated regions.
Youwei Hong, Keran Zhang, Dan Liao, Gaojie Chen, Min Zhao, Yiling Lin, Xiaoting Ji, Ke Xu, Yu Wu, Ruilian Yu, Gongren Hu, Sung-Deuk Choi, Likun Xue, and Jinsheng Chen
EGUsphere, https://doi.org/10.5194/egusphere-2023-1242, https://doi.org/10.5194/egusphere-2023-1242, 2023
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Particle uptakes of HCHO and the impacts on PM2.5 and O3 production remain highly uncertain. Based on the investigation of co-occurring wintertime O3 and PM2.5 pollution in a coastal city of southeast China, we found enhanced the heterogeneous formation of hydroxymethanesulfonate (HMS), and increased the ROx concentrations and net O3 production rates. The findings of this study are helpful to better explore the mechanisms of key precursors for co-occurring PM2.5 and O3 pollution.
Haeyoung Lee, Wonick Seo, Shanlan Li, Soojeong Lee, Samuel Takele Kenea, and Sangwon Joo
Atmos. Chem. Phys., 23, 7141–7159, https://doi.org/10.5194/acp-23-7141-2023, https://doi.org/10.5194/acp-23-7141-2023, 2023
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We introduced three Korea Meteorological Administration (KMA) monitoring stations with monitoring systems and measurement uncertainty. We also analyzed the regional characteristics of CH4 at each KMA station. CH4 levels measured at KMA stations are compared to those measured at other Asian stations. From the long-term records of CH4 and δ13CH4 at AMY, we confirmed that the source of CH4xs changed from the past (2006 to 2010) to recent (2016 to 2020) years in East Asia.
Robert G. Ryan, Eloise A. Marais, Eleanor Gershenson-Smith, Robbie Ramsay, Jan-Peter Muller, Jan-Lukas Tirpitz, and Udo Frieß
Atmos. Chem. Phys., 23, 7121–7139, https://doi.org/10.5194/acp-23-7121-2023, https://doi.org/10.5194/acp-23-7121-2023, 2023
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We describe the first data retrieval from a newly installed instrument providing measurements of vertical profiles of air pollution over Central London during heatwaves in summer 2022. We use these observations with surface air quality network measurements to support interpretation that an exponential increase in biogenic emissions of isoprene during heatwaves provides the limiting ingredient for severe ozone pollution, leading to non-compliance with the national ozone air quality standard.
Zhouxing Zou, Qianjie Chen, Men Xia, Qi Yuan, Yi Chen, Yanan Wang, Enyu Xiong, Zhe Wang, and Tao Wang
Atmos. Chem. Phys., 23, 7057–7074, https://doi.org/10.5194/acp-23-7057-2023, https://doi.org/10.5194/acp-23-7057-2023, 2023
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We present OH observation and model simulation results at a coastal site in Hong Kong. The model predicted the OH concentration under high-NOx well but overpredicted it under low-NOx conditions. This implies an insufficient understanding of OH chemistry under low-NOx conditions. We show evidence of missing OH sinks as a possible cause of the overprediction.
Yaqin Gao, Hongli Wang, Lingling Yuan, Shengao Jing, Bin Yuan, Guofeng Shen, Liang Zhu, Abigail Koss, Yingjie Li, Qian Wang, Dan Dan Huang, Shuhui Zhu, Shikang Tao, Shengrong Lou, and Cheng Huang
Atmos. Chem. Phys., 23, 6633–6646, https://doi.org/10.5194/acp-23-6633-2023, https://doi.org/10.5194/acp-23-6633-2023, 2023
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A near-complete speciation of reactive organic gases from residential combustion was developed to get more insights into their atmospheric effects. Oxygenated species, higher hydrocarbons and nitrogen-containing species played larger roles in these emissions compared with common hydrocarbons. Based on the near-complete speciation, these emissions were largely underestimated, leading to more underestimation of their hydroxyl radical reactivity and secondary organic aerosol formation potential.
Jinsol Kim, John B. Miller, Charles E. Miller, Scott J. Lehman, Sylvia E. Michel, Vineet Yadav, Nick E. Rollins, and William M. Berelson
EGUsphere, https://doi.org/10.5194/egusphere-2023-957, https://doi.org/10.5194/egusphere-2023-957, 2023
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In this study, we present the partitioning of CO2 signals from biogenic, petroleum and natural gas sources by combining CO, δ13CO2, and Δ14CO2 measurements. Using measurements from flask air samples at three sites in the greater Los Angels region, we find larger and positive contributions of biogenic signals in winter and smaller and negative contributions in summer. Largest contribution of natural gas combustion generally occurs in summer.
Zaneta Hamryszczak, Dirk Dienhart, Bettina Brendel, Roland Rohloff, Daniel Marno, Monica Martinez, Hartwig Harder, Andrea Pozzer, Birger Bohn, Martin Zöger, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 23, 5929–5943, https://doi.org/10.5194/acp-23-5929-2023, https://doi.org/10.5194/acp-23-5929-2023, 2023
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Hydrogen peroxide is a key contributor to the oxidative chemistry of the atmosphere through its link to the most prominent oxidants controlling its self-cleansing capacity, HOx. During the CAFE-Africa campaign, H2O2 was measured over the Atlantic Ocean and western Africa in August/September 2018. The study gives an overview of the distribution of H2O2 in the upper tropical troposphere and investigates the impact of convective processes in the Intertropical Convergence Zone on the budget of H2O2.
Chengzhi Xing, Shiqi Xu, Yuhang Song, Cheng Liu, Yuhan Liu, Keding Lu, Wei Tan, Chengxin Zhang, Qihou Hu, Shanshan Wang, Hongyu Wu, and Hua Lin
Atmos. Chem. Phys., 23, 5815–5834, https://doi.org/10.5194/acp-23-5815-2023, https://doi.org/10.5194/acp-23-5815-2023, 2023
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High RH could contribute to the secondary formation of HONO in the sea atmosphere. High temperature could promote the formation of HONO from NO2 heterogeneous reactions in the sea and coastal atmosphere. The aerosol surface plays a more important role during the above process in coastal and sea cases. The generation rate of HONO from the NO2 heterogeneous reaction in the sea cases is larger than that in inland cases in higher atmospheric layers above 600 m.
Daniel John Katz, Aroob Abdelhamid, Harald Stark, Manjula R. Canagaratna, Douglas R. Worsnop, and Eleanor C. Browne
Atmos. Chem. Phys., 23, 5567–5585, https://doi.org/10.5194/acp-23-5567-2023, https://doi.org/10.5194/acp-23-5567-2023, 2023
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Ambient ion chemical composition measurements provide insight into trace gases that are precursors for the formation and growth of new aerosol particles. We use a new data analysis approach to increase the chemical information from these measurements. We analyze results from an agricultural region, a little studied land use type that is ~41 % of global land use, and find that the composition of gases important for aerosol formation and growth differs significantly from that in other ecosystems.
Amelia M. H. Bond, Markus M. Frey, Jan Kaiser, Jörg Kleffmann, Anna E. Jones, and Freya A. Squires
Atmos. Chem. Phys., 23, 5533–5550, https://doi.org/10.5194/acp-23-5533-2023, https://doi.org/10.5194/acp-23-5533-2023, 2023
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Atmospheric nitrous acid (HONO) amount fractions measured at Halley Research Station, Antarctica, were found to be low. Vertical fluxes of HONO from the snow were also measured and agree with the estimated HONO production rate from photolysis of snow nitrate. In a simple box model of HONO sources and sinks, there was good agreement between the measured flux and amount fraction. HONO was found to be an important OH radical source at Halley.
Rujing Yin, Xiaoxiao Li, Chao Yan, Runlong Cai, Ying Zhou, Juha Kangasluoma, Nina Sarnela, Janne Lampilahti, Tuukka Petäjä, Veli-Matti Kerminen, Federico Bianchi, Markku Kulmala, and Jingkun Jiang
Atmos. Chem. Phys., 23, 5279–5296, https://doi.org/10.5194/acp-23-5279-2023, https://doi.org/10.5194/acp-23-5279-2023, 2023
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Atmospheric cluster ions are important constituents in the atmosphere. However, the quantitative research on their compositions is still limited, especially in urban environments. Here we demonstrate the feasibility of an in situ quantification method of cluster ions measured by a high-resolution mass spectrometer and reveal their governing factors, sources, and sinks in urban Beijing through quantitative analysis of cluster ions, reagent ions, neutral molecules, and condensation sink.
Magdalena Okuljar, Olga Garmash, Miska Olin, Joni Kalliokoski, Hilkka Timonen, Jarkko V. Niemi, Pauli Paasonen, Jenni Kontkanen, Yanjun Zhang, Heidi Hellén, Heino Kuuluvainen, Minna Aurela, Hanna E. Manninen, Mikko Sipilä, Topi Rönkkö, Tuukka Petäjä, Markku Kulmala, Miikka Dal Maso, and Mikael Ehn
EGUsphere, https://doi.org/10.5194/egusphere-2023-524, https://doi.org/10.5194/egusphere-2023-524, 2023
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Highly oxygenated organic molecules form secondary organic aerosol that affects air quality and health. In this study, we demonstrate that in a moderately polluted city with abundant vegetation, the composition of HOM is largely controlled by the effect of NOx on the biogenic VOC oxidation. Comparing the results from two nearby stations, we show that HOM composition and formation pathways can change considerably within small distances in urban environments.
Eva Y. Pfannerstill, Caleb Arata, Qindan Zhu, Benjamin C. Schulze, Roy Woods, John H. Seinfeld, Anthony Bucholtz, Ronald C. Cohen, and Allen H. Goldstein
EGUsphere, https://doi.org/10.5194/egusphere-2023-723, https://doi.org/10.5194/egusphere-2023-723, 2023
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The San Joaquin Valley is an agricultural area with poor air quality. Organic gases drive the formation of hazardous air pollutants. Agricultural emissions of these gases are not well understood and have rarely been quantified at landscape scale. By combining aircraft-based emission measurements with land cover information, we found mis- or unrepresented emission sources. The results of this study help understand pollution sources and improve predictions of air quality in agricultural regions.
Qiaozhi Zha, Wei Huang, Diego Aliaga, Otso Peräkylä, Liine Heikkinen, Alkuin Maximilian Koenig, Cheng Wu, Joonas Enroth, Yvette Gramlich, Jing Cai, Samara Carbone, Armin Hansel, Tuukka Petäjä, Markku Kulmala, Douglas Worsnop, Victoria Sinclair, Radovan Krejci, Marcos Andrade, Claudia Mohr, and Federico Bianchi
Atmos. Chem. Phys., 23, 4559–4576, https://doi.org/10.5194/acp-23-4559-2023, https://doi.org/10.5194/acp-23-4559-2023, 2023
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We investigate the chemical composition of atmospheric cluster ions from January to May 2018 at the high-altitude research station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes. With state-of-the-art mass spectrometers and air mass history analysis, the measured cluster ions exhibited distinct diurnal and seasonal patterns, some of which contributed to new particle formation. Our study will improve the understanding of atmospheric ions and their role in high-altitude new particle formation.
Zeyu Sun, Zheng Zong, Yang Tan, Chongguo Tian, Zeyu Liu, Fan Zhang, Rong Sun, Yingjun Chen, Jun Li, and Gan Zhang
EGUsphere, https://doi.org/10.5194/egusphere-2023-500, https://doi.org/10.5194/egusphere-2023-500, 2023
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This is the first report of ship-emitted nitrogen stable isotope composition (δ15N) of nitrogen oxides (NOx). Results showed that δ15N–NOx from ships was −18.5 ± 10.9 ‰ and increased monotonically with tightening emission regulations. The selective catalytic reduction system was the most vital factor. The temporal variation in δ15N–NOx was evaluated and can be used to select suitable δ15N–NOx for a more accurate assessment of the contribution of ship-emitted exhaust to atmospheric NOx.
Clara M. Nussbaumer, Bryan K. Place, Qindan Zhu, Eva Y. Pfannerstill, Paul Wooldridge, Benjamin C. Schulze, Caleb Arata, Ryan Ward, Anthony Bucholtz, John H. Seinfeld, Allen H. Goldstein, and Ronald C. Cohen
EGUsphere, https://doi.org/10.5194/egusphere-2023-601, https://doi.org/10.5194/egusphere-2023-601, 2023
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NOx is a precursor to hazardous tropospheric ozone and can be emitted from various anthropogenic sources. It is important to quantify NOx emissions in urban environments in order to improve the local air quality which still remains a challenge as sources are heterogeneous in space and time. In this study, we calculate NOx emissions over Los Angeles based on aircraft measurements in June 2021 and compare them to a local emission inventory which we find to mostly overpredict the measured values.
Michael P. Vermeuel, Gordon A. Novak, Delaney B. Kilgour, Megan S. Claflin, Brian M. Lerner, Amy M. Trowbridge, Jonathan Thom, Patricia A. Cleary, Ankur R. Desai, and Timothy H. Bertram
Atmos. Chem. Phys., 23, 4123–4148, https://doi.org/10.5194/acp-23-4123-2023, https://doi.org/10.5194/acp-23-4123-2023, 2023
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Reactive carbon species emitted from natural sources such as forests play an important role in the chemistry of the atmosphere. Predictions of these emissions are based on plant responses during the growing season and do not consider potential effects from seasonal changes. To address this, we made measurements of reactive carbon over a forest during the summer to autumn transition. We learned that observed concentrations and emissions for some key species are larger than model predictions.
Huiming Lin, Yindong Tong, Long Chen, Chenghao Yu, Zhaohan Chu, Qianru Zhang, Xiufeng Yin, Qianggong Zhang, Shichang Kang, Junfeng Liu, James Schauer, Benjamin de Foy, and Xuejun Wang
Atmos. Chem. Phys., 23, 3937–3953, https://doi.org/10.5194/acp-23-3937-2023, https://doi.org/10.5194/acp-23-3937-2023, 2023
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Lhasa is the largest city in the Tibetan Plateau, and its atmospheric mercury concentrations represent the highest level of pollution in this region. Unexpectedly high concentrations of atmospheric mercury species were found. Combined with the trajectory analysis, the high atmospheric mercury concentrations may have originated from external long-range transport. Local sources, especially special mercury-related sources, are important factors influencing the variability of atmospheric mercury.
Vaishali Jain, Nidhi Tripathi, Sachchida N. Tripathi, Mansi Gupta, Lokesh K. Sahu, Vishnu Murari, Sreenivas Gaddamidi, Ashutosh K. Shukla, and Andre S. H. Prevot
Atmos. Chem. Phys., 23, 3383–3408, https://doi.org/10.5194/acp-23-3383-2023, https://doi.org/10.5194/acp-23-3383-2023, 2023
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This research chemically characterises 173 different NMVOCs (non-methane volatile organic compounds) measured in real time for three seasons in the city of the central Indo-Gangetic basin of India, Lucknow. Receptor modelling is used to analyse probable sources of NMVOCs and their crucial role in forming ozone and secondary organic aerosols. It is observed that vehicular emissions and solid fuel combustion are the highest contributors to the emission of primary and secondary NMVOCs.
Yizhen Wu, Juntao Huo, Gan Yang, Yuwei Wang, Lihong Wang, Shijian Wu, Lei Yao, Qingyan Fu, and Lin Wang
Atmos. Chem. Phys., 23, 2997–3014, https://doi.org/10.5194/acp-23-2997-2023, https://doi.org/10.5194/acp-23-2997-2023, 2023
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Based on a field campaign in a suburban area of Shanghai during summer 2021, we calculated formaldehyde (HCHO) production rates from 24 volatile organic compounds (VOCs). In addition, HCHO photolysis, reactions with OH radicals, and dry deposition were considered for the estimation of HCHO loss rates. Our results reveal the key precursors of HCHO and suggest that HCHO wet deposition may be an important loss term on cloudy and rainy days, which needs to be further investigated.
Yu Han, Tao Wang, Rui Li, Hongbo Fu, Yusen Duan, Song Gao, Liwu Zhang, and Jianmin Chen
Atmos. Chem. Phys., 23, 2877–2900, https://doi.org/10.5194/acp-23-2877-2023, https://doi.org/10.5194/acp-23-2877-2023, 2023
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Limited knowledge is available on volatile organic compound (VOC) multi-site research of different land-use types at city level. This study performed a concurrent multi-site observation campaign on the three typical land-use types of Shanghai, East China. The results showed that concentrations, sources and ozone and secondary organic aerosol formation potentials of VOCs varied with the land-use types.
Zhensen Zheng, Kangwei Li, Bo Xu, Jianping Dou, Liming Li, Guotao Zhang, Shijie Li, Chunmei Geng, Wen Yang, Merched Azzi, and Zhipeng Bai
Atmos. Chem. Phys., 23, 2649–2665, https://doi.org/10.5194/acp-23-2649-2023, https://doi.org/10.5194/acp-23-2649-2023, 2023
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Previous box model studies applied different timescales of observational datasets to identify the O3–precursor relationship, but there is a lack of comparison among these different timescales regarding the impact of O3 formation chemistry. Through a case study at Zibo in China, we find that the O3 formation regime showed overall consistency but non-negligible variability among various patterns of timescale. This would be complementary in developing more accurate O3 pollution control strategies.
Lejish Vettikkat, Pasi Miettinen, Angela Buchholz, Pekka Rantala, Hao Yu, Simon Schallhart, Tuukka Petäjä, Roger Seco, Elisa Männistö, Markku Kulmala, Eeva-Stiina Tuittila, Alex B. Guenther, and Siegfried Schobesberger
Atmos. Chem. Phys., 23, 2683–2698, https://doi.org/10.5194/acp-23-2683-2023, https://doi.org/10.5194/acp-23-2683-2023, 2023
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Wetlands cover a substantial fraction of the land mass in the northern latitudes, from northern Europe to Siberia and Canada. Yet, their isoprene and terpene emissions remain understudied. Here, we used a state-of-the-art measurement technique to quantify ecosystem-scale emissions from a boreal wetland during an unusually warm spring/summer. We found that the emissions from this wetland were (a) higher and (b) even more strongly dependent on temperature than commonly thought.
Tianyu Zhai, Keding Lu, Haichao Wang, Shengrong Lou, Xiaorui Chen, Renzhi Hu, and Yuanhang Zhang
Atmos. Chem. Phys., 23, 2379–2391, https://doi.org/10.5194/acp-23-2379-2023, https://doi.org/10.5194/acp-23-2379-2023, 2023
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Particulate nitrate is a growing issue in air pollution. Based on comprehensive field measurement, we show heavy nitrate pollution in eastern China in summer. OH reacting with NO2 at daytime dominates nitrate formation on clean days, while N2O5 hydrolysis largely enhances and become comparable with that of OH reacting with O2 on polluted days (67.2 % and 30.2 %). Model simulation indicates that VOC : NOx = 2 : 1 is effective in mitigating the O3 and nitrate pollution coordinately.
Samuel J. Cliff, Will Drysdale, James D. Lee, Carole Helfter, Eiko Nemitz, Stefan Metzger, and Janet F. Barlow
Atmos. Chem. Phys., 23, 2315–2330, https://doi.org/10.5194/acp-23-2315-2023, https://doi.org/10.5194/acp-23-2315-2023, 2023
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Emissions of nitrogen oxides (NOx) to the atmosphere are an ongoing air quality issue. This study directly measures emissions of NOx and carbon dioxide from a tall tower in central London during the coronavirus pandemic. It was found that transport NOx emissions had reduced by >73 % since 2017 as a result of air quality policy and reduced congestion during coronavirus restrictions. During this period, central London was thought to be dominated by point-source heat and power generation emissions.
Laura Tomsche, Felix Piel, Tomas Mikoviny, Claus J. Nielsen, Hongyu Guo, Pedro Campuzano-Jost, Benjamin A. Nault, Melinda K. Schueneman, Jose L. Jimenez, Hannah Halliday, Glenn Diskin, Joshua P. DiGangi, John B. Nowak, Elizabeth B. Wiggins, Emily Gargulinski, Amber J. Soja, and Armin Wisthaler
Atmos. Chem. Phys., 23, 2331–2343, https://doi.org/10.5194/acp-23-2331-2023, https://doi.org/10.5194/acp-23-2331-2023, 2023
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Ammonia (NH3) is an important trace gas in the atmosphere and fires are among the poorly investigated sources. During the 2019 Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) aircraft campaign, we measured gaseous NH3 and particulate ammonium (NH4+) in smoke plumes emitted from 6 wildfires in the Western US and 66 small agricultural fires in the Southeastern US. We herein present a comprehensive set of emission factors of NH3 and NHx, where NHx = NH3 + NH4+.
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.
Eric Förster, Harald Bönisch, Marco Neumaier, Florian Obersteiner, Andreas Zahn, Andreas Hilboll, Anna B. Kalisz Hedegaard, Nikos Daskalakis, Alexandros Panagiotis Poulidis, Mihalis Vrekoussis, Michael Lichtenstern, and Peter Braesicke
Atmos. Chem. Phys., 23, 1893–1918, https://doi.org/10.5194/acp-23-1893-2023, https://doi.org/10.5194/acp-23-1893-2023, 2023
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The airborne megacity campaign EMeRGe provided an unprecedented amount of trace gas measurements. We combine measured volatile organic compounds (VOCs) with trajectory-modelled emission uptakes to identify potential source regions of pollution. We also characterise the chemical fingerprints (e.g. biomass burning and anthropogenic signatures) of the probed air masses to corroborate the contributing source regions. Our approach is the first large-scale study of VOCs originating from megacities.
Jacob T. Shaw, Amy Foulds, Shona Wilde, Patrick Barker, Freya A. Squires, James Lee, Ruth Purvis, Ralph Burton, Ioana Colfescu, Stephen Mobbs, Samuel Cliff, Stéphane J.-B. Bauguitte, Stuart Young, Stefan Schwietzke, and Grant Allen
Atmos. Chem. Phys., 23, 1491–1509, https://doi.org/10.5194/acp-23-1491-2023, https://doi.org/10.5194/acp-23-1491-2023, 2023
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Flaring is used by the oil and gas sector to dispose of unwanted natural gas or for safety. However, few studies have assessed the efficiency with which the gas is combusted. We sampled flaring emissions from offshore facilities in the North Sea. Average measured flaring efficiencies were ~ 98 % but with a skewed distribution, including many flares of lower efficiency. NOx and ethane emissions were also measured. Inefficient flaring practices could be a target for mitigating carbon emissions.
Wiebke Scholz, Jiali Shen, Diego Aliaga, Cheng Wu, Samara Carbone, Isabel Moreno, Qiaozhi Zha, Wei Huang, Liine Heikkinen, Jean Luc Jaffrezo, Gaelle Uzu, Eva Partoll, Markus Leiminger, Fernando Velarde, Paolo Laj, Patrick Ginot, Paolo Artaxo, Alfred Wiedensohler, Markku Kulmala, Claudia Mohr, Marcos Andrade, Victoria Sinclair, Federico Bianchi, and Armin Hansel
Atmos. Chem. Phys., 23, 895–920, https://doi.org/10.5194/acp-23-895-2023, https://doi.org/10.5194/acp-23-895-2023, 2023
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Dimethyl sulfide (DMS), emitted from the ocean, is the most abundant biogenic sulfur emission into the atmosphere. OH radicals, among others, can oxidize DMS to sulfuric and methanesulfonic acid, which are relevant for aerosol formation. We quantified DMS and nearly all DMS oxidation products with novel mass spectrometric instruments for gas and particle phase at the high mountain station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes in free tropospheric air after long-range transport.
Magdalena Pühl, Anke Roiger, Alina Fiehn, Alan M. Gorchov Negron, Eric A. Kort, Stefan Schwietzke, Ignacio Pisso, Amy Foulds, James Lee, James L. France, Anna E. Jones, Dave Lowry, Rebecca E. Fisher, Langwen Huang, Jacob Shaw, Prudence Bateson, Stephen Andrews, Stuart Young, Pamela Dominutti, Tom Lachlan-Cope, Alexandra Weiss, and Grant Allen
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-826, https://doi.org/10.5194/acp-2022-826, 2023
Revised manuscript accepted for ACP
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In April–May 2019 we carried out an airborne field campaign in the Southern North Sea with the aim to study methane emissions of offshore gas installations. We determine methane emissions from elevated methane measured downstream of the sampled installations. We compare our measured methane emissions with estimated methane emissions from national and global annual inventories. As a result, we find inconsistencies of inventories and large discrepancies between measurements and inventories.
Dirk Dienhart, Bettina Brendel, John N. Crowley, Philipp G. Eger, Hartwig Harder, Monica Martinez, Andrea Pozzer, Roland Rohloff, Jan Schuladen, Sebastian Tauer, David Walter, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 23, 119–142, https://doi.org/10.5194/acp-23-119-2023, https://doi.org/10.5194/acp-23-119-2023, 2023
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Formaldehyde and hydroperoxide measurements were performed in the marine boundary layer around the Arabian Peninsula and highlight the Suez Canal and Arabian (Persian) Gulf as a hotspot of photochemical air pollution. A comparison with the EMAC model shows that the formaldehyde results match within a factor of 2, while hydrogen peroxide was overestimated by more than a factor of 5, which revealed enhanced HOx (OH+HO2) radicals in the simulation and an underestimation of dry deposition velocites.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven C. Wofsy
Atmos. Chem. Phys., 23, 99–117, https://doi.org/10.5194/acp-23-99-2023, https://doi.org/10.5194/acp-23-99-2023, 2023
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We have prepared a unique and unusual result from the recent ATom aircraft mission: a measurement-based derivation of the production and loss rates of ozone and methane over the ocean basins. These are the key products of chemistry models used in assessments but have thus far lacked observational metrics. It also shows the scales of variability of atmospheric chemical rates and provides a major challenge to the atmospheric models.
Simone T. Andersen, Beth S. Nelson, Katie A. Read, Shalini Punjabi, Luis Neves, Matthew J. Rowlinson, James Hopkins, Tomás Sherwen, Lisa K. Whalley, James D. Lee, and Lucy J. Carpenter
Atmos. Chem. Phys., 22, 15747–15765, https://doi.org/10.5194/acp-22-15747-2022, https://doi.org/10.5194/acp-22-15747-2022, 2022
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The cycling of NO and NO2 is important to understand to be able to predict O3 concentrations in the atmosphere. We have used long-term measurements from the Cape Verde Atmospheric Observatory together with model outputs to investigate the cycling of nitrogen oxide (NO) and nitrogen dioxide (NO2) in very clean marine air. This study shows that we understand the processes occurring in very clean air, but with small amounts of pollution in the air, known chemistry cannot explain what is observed.
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