Articles | Volume 21, issue 23
https://doi.org/10.5194/acp-21-17373-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-21-17373-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Measurement report
| 
01 Dec 2021
Measurement report |
| 01 Dec 2021
| 01 Dec 2021
Measurement report: Observation-based formaldehyde production rates and their relation to OH reactivity around the Arabian Peninsula
Department of Atmospheric Chemistry, Max Planck Institute for Chemistry, Mainz, Germany
John N. Crowley
Department of Atmospheric Chemistry, Max Planck Institute for Chemistry, Mainz, Germany
Efstratios Bourtsoukidis
Climate and Atmosphere Research Centre, The Cyprus Institute, Nicosia, Cyprus
Achim Edtbauer
Department of Atmospheric Chemistry, Max Planck Institute for Chemistry, Mainz, Germany
Philipp G. Eger
Department of Atmospheric Chemistry, Max Planck Institute for Chemistry, Mainz, Germany
Lisa Ernle
Department of Atmospheric Chemistry, Max Planck Institute for Chemistry, Mainz, Germany
Hartwig Harder
Department of Atmospheric Chemistry, Max Planck Institute for Chemistry, Mainz, Germany
Bettina Hottmann
Department of Atmospheric Chemistry, Max Planck Institute for Chemistry, Mainz, Germany
Monica Martinez
Department of Atmospheric Chemistry, Max Planck Institute for Chemistry, Mainz, Germany
Uwe Parchatka
Department of Atmospheric Chemistry, Max Planck Institute for Chemistry, Mainz, Germany
Jean-Daniel Paris
Laboratoire des Sciences du Climat et de l'Environnement, CEA-CNRS-UVSQ, UMR8212, IPSL, Gif-sur-Yvette, France
Climate and Atmosphere Research Centre, The Cyprus Institute, Nicosia, Cyprus
Eva Y. Pfannerstill
Department of Atmospheric Chemistry, Max Planck Institute for Chemistry, Mainz, Germany
Roland Rohloff
Department of Atmospheric Chemistry, Max Planck Institute for Chemistry, Mainz, Germany
Jan Schuladen
Department of Atmospheric Chemistry, Max Planck Institute for Chemistry, Mainz, Germany
Christof Stönner
Department of Atmospheric Chemistry, Max Planck Institute for Chemistry, Mainz, Germany
Ivan Tadic
Department of Atmospheric Chemistry, Max Planck Institute for Chemistry, Mainz, Germany
Sebastian Tauer
Department of Atmospheric Chemistry, Max Planck Institute for Chemistry, Mainz, Germany
Nijing Wang
Department of Atmospheric Chemistry, Max Planck Institute for Chemistry, Mainz, Germany
Jonathan Williams
Department of Atmospheric Chemistry, Max Planck Institute for Chemistry, Mainz, Germany
Climate and Atmosphere Research Centre, The Cyprus Institute, Nicosia, Cyprus
Jos Lelieveld
Department of Atmospheric Chemistry, Max Planck Institute for Chemistry, Mainz, Germany
Climate and Atmosphere Research Centre, The Cyprus Institute, Nicosia, Cyprus
Horst Fischer
CORRESPONDING AUTHOR
Department of Atmospheric Chemistry, Max Planck Institute for Chemistry, Mainz, Germany
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Pantelis Georgiades, Matthias Kohl, Mihalis A. Nicolaou, Theodoros Christoudias, Andrea Pozzer, Constantine Dovrolis, and Jos Lelieveld
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2024-314, https://doi.org/10.5194/essd-2024-314, 2024
Manuscript not accepted for further review
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Anna Martin, Veronika Gayler, Benedikt Steil, Klaus Klingmüller, Patrick Jöckel, Holger Tost, Jos Lelieveld, and Andrea Pozzer
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Atmos. Chem. Phys., 24, 7499–7522, https://doi.org/10.5194/acp-24-7499-2024, https://doi.org/10.5194/acp-24-7499-2024, 2024
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Georgia Lazoglou, Theo Economou, Christina Anagnostopoulou, George Zittis, Anna Tzyrkalli, Pantelis Georgiades, and Jos Lelieveld
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Linda Ort, Lenard Lukas Röder, Uwe Parchatka, Rainer Königstedt, Daniel Crowley, Frank Kunz, Ralf Wittkowski, Jos Lelieveld, and Horst Fischer
Atmos. Meas. Tech., 17, 3553–3565, https://doi.org/10.5194/amt-17-3553-2024, https://doi.org/10.5194/amt-17-3553-2024, 2024
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Atmos. Chem. Phys., 24, 6359–6373, https://doi.org/10.5194/acp-24-6359-2024, https://doi.org/10.5194/acp-24-6359-2024, 2024
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Atmos. Chem. Phys., 24, 5265–5286, https://doi.org/10.5194/acp-24-5265-2024, https://doi.org/10.5194/acp-24-5265-2024, 2024
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Volatile organic compounds (VOCs) fuel the production of air pollutants like ozone and particulate matter. The representation of VOC chemistry remains challenging due to its complexity in speciation and reactions. Here, we develop a chemical mechanism, RACM2B-VCP, that better represents VOC chemistry in urban areas such as Los Angeles. We also discuss the contribution of VOCs emitted from volatile chemical products and other anthropogenic sources to total VOC reactivity and O3.
Yunsong Liu, Jean-Daniel Paris, Gregoire Broquet, Violeta Bescós Roy, Tania Meixus Fernandez, Rasmus Andersen, Andrés Russu Berlanga, Emil Christensen, Yann Courtois, Sebastian Dominok, Corentin Dussenne, Travis Eckert, Andrew Finlayson, Aurora Fernández de la Fuente, Catlin Gunn, Ram Hashmonay, Juliano Grigoleto Hayashi, Jonathan Helmore, Soeren Honsel, Fabrizio Innocenti, Matti Irjala, Torgrim Log, Cristina Lopez, Francisco Cortés Martínez, Jonathan Martinez, Adrien Massardier, Helle Gottschalk Nygaard, Paula Agregan Reboredo, Elodie Rousset, Axel Scherello, Matthias Ulbricht, Damien Weidmann, Oliver Williams, Nigel Yarrow, Murès Zarea, Robert Ziegler, Jean Sciare, Mihalis Vrekoussis, and Philippe Bousquet
Atmos. Meas. Tech., 17, 1633–1649, https://doi.org/10.5194/amt-17-1633-2024, https://doi.org/10.5194/amt-17-1633-2024, 2024
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Pramod Kumar, Christopher Caldow, Grégoire Broquet, Adil Shah, Olivier Laurent, Camille Yver-Kwok, Sebastien Ars, Sara Defratyka, Susan Warao Gichuki, Luc Lienhardt, Mathis Lozano, Jean-Daniel Paris, Felix Vogel, Caroline Bouchet, Elisa Allegrini, Robert Kelly, Catherine Juery, and Philippe Ciais
Atmos. Meas. Tech., 17, 1229–1250, https://doi.org/10.5194/amt-17-1229-2024, https://doi.org/10.5194/amt-17-1229-2024, 2024
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This study presents a series of mobile measurement campaigns to monitor the CH4 emissions from an active landfill. These measurements are processed using a Gaussian plume model and atmospheric inversion techniques to quantify the landfill CH4 emissions. The methane emission estimates range between ~0.4 and ~7 t CH4 per day, and their variations are analyzed. The robustness of the estimates is assessed depending on the distance of the measurements from the potential sources in the landfill.
Imran A. Girach, Narendra Ojha, Prabha R. Nair, Kandula V. Subrahmanyam, Neelakantan Koushik, Mohammed M. Nazeer, Nadimpally Kiran Kumar, Surendran Nair Suresh Babu, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 24, 1979–1995, https://doi.org/10.5194/acp-24-1979-2024, https://doi.org/10.5194/acp-24-1979-2024, 2024
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We investigate surface ozone variability in East Antarctica based on measurements and EMAC global model simulations during austral summer. Nearly half of the surface ozone is found to be of stratospheric origin. The east coast of Antarctica acts as a stronger sink of ozone than surrounding regions. Photochemical loss of ozone is counterbalanced by downward transport of ozone. The study highlights the intertwined role of chemistry and dynamics in governing ozone variations over East Antarctica.
Matthew M. Coggon, Chelsea E. Stockwell, Megan S. Claflin, Eva Y. Pfannerstill, Lu Xu, Jessica B. Gilman, Julia Marcantonio, Cong Cao, Kelvin Bates, Georgios I. Gkatzelis, Aaron Lamplugh, Erin F. Katz, Caleb Arata, Eric C. Apel, Rebecca S. Hornbrook, Felix Piel, Francesca Majluf, Donald R. Blake, Armin Wisthaler, Manjula Canagaratna, Brian M. Lerner, Allen H. Goldstein, John E. Mak, and Carsten Warneke
Atmos. Meas. Tech., 17, 801–825, https://doi.org/10.5194/amt-17-801-2024, https://doi.org/10.5194/amt-17-801-2024, 2024
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Mass spectrometry is a tool commonly used to measure air pollutants. This study evaluates measurement artifacts produced in the proton-transfer-reaction mass spectrometer. We provide methods to correct these biases and better measure compounds that degrade air quality.
Ryan Vella, Andrea Pozzer, Matthew Forrest, Jos Lelieveld, Thomas Hickler, and Holger Tost
Biogeosciences, 20, 4391–4412, https://doi.org/10.5194/bg-20-4391-2023, https://doi.org/10.5194/bg-20-4391-2023, 2023
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We investigated the effect of the El Niño–Southern Oscillation (ENSO) on biogenic volatile organic compound (BVOC) emissions from plants. ENSO events can cause a significant increase in these emissions, which have a long-term impact on the Earth's atmosphere. Persistent ENSO conditions can cause long-term changes in vegetation, resulting in even higher BVOC emissions. We link ENSO-induced emission anomalies with driving atmospheric and vegetational variables.
Susanna Strada, Andrea Pozzer, Graziano Giuliani, Erika Coppola, Fabien Solmon, Xiaoyan Jiang, Alex Guenther, Efstratios Bourtsoukidis, Dominique Serça, Jonathan Williams, and Filippo Giorgi
Atmos. Chem. Phys., 23, 13301–13327, https://doi.org/10.5194/acp-23-13301-2023, https://doi.org/10.5194/acp-23-13301-2023, 2023
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Water deficit modifies emissions of isoprene, an aromatic compound released by plants that influences the production of an air pollutant such as ozone. Numerical modelling shows that, during the warmest and driest summers, isoprene decreases between −20 and −60 % over the Euro-Mediterranean region, while near-surface ozone only diminishes by a few percent. Decreases in isoprene emissions not only happen under dry conditions, but also could occur after prolonged or repeated water deficits.
Zaneta Hamryszczak, Antonia Hartmann, Dirk Dienhart, Sascha Hafermann, Bettina Brendel, Rainer Königstedt, Uwe Parchatka, Jos Lelieveld, and Horst Fischer
Atmos. Meas. Tech., 16, 4741–4756, https://doi.org/10.5194/amt-16-4741-2023, https://doi.org/10.5194/amt-16-4741-2023, 2023
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Hydroperoxide measurements improve the understanding of atmospheric oxidation processes. We introduce an instrumental setup for airborne measurements. The aim of the work is the characterization of the measurement method with emphasis on interferences impacting instrumental uncertainty. Technical and physical challenges do not critically impact the instrumental performance. The instrument resolves dynamic processes, such as convective transport, as shown based on the CAFE-Brazil campaign.
Matthias Kohl, Jos Lelieveld, Sourangsu Chowdhury, Sebastian Ehrhart, Disha Sharma, Yafang Cheng, Sachchida Nand Tripathi, Mathew Sebastian, Govindan Pandithurai, Hongli Wang, and Andrea Pozzer
Atmos. Chem. Phys., 23, 13191–13215, https://doi.org/10.5194/acp-23-13191-2023, https://doi.org/10.5194/acp-23-13191-2023, 2023
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Knowledge on atmospheric ultrafine particles (UFPs) with a diameter smaller than 100 nm is crucial for public health and the hydrological cycle. We present a new global dataset of UFP concentrations at the Earth's surface derived with a comprehensive chemistry–climate model and evaluated with ground-based observations. The evaluation results are combined with high-resolution primary emissions to downscale UFP concentrations to an unprecedented horizontal resolution of 0.1° × 0.1°.
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
Atmos. Chem. Phys., 23, 13015–13028, https://doi.org/10.5194/acp-23-13015-2023, https://doi.org/10.5194/acp-23-13015-2023, 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 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 mostly overpredicts the measured values.
Eva Y. Pfannerstill, Caleb Arata, Qindan Zhu, Benjamin C. Schulze, Roy Woods, John H. Seinfeld, Anthony Bucholtz, Ronald C. Cohen, and Allen H. Goldstein
Atmos. Chem. Phys., 23, 12753–12780, https://doi.org/10.5194/acp-23-12753-2023, https://doi.org/10.5194/acp-23-12753-2023, 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. Our results help in understanding of pollution sources and in improving predictions of air quality in agricultural regions.
Clara M. Nussbaumer, Horst Fischer, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 23, 12651–12669, https://doi.org/10.5194/acp-23-12651-2023, https://doi.org/10.5194/acp-23-12651-2023, 2023
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Ozone is a greenhouse gas and contributes to the earth’s radiative energy budget and therefore to global warming. This effect is the largest in the upper troposphere. In this study, we investigate the processes controlling ozone formation and the sensitivity to its precursors in the upper tropical troposphere based on model simulations by the ECHAM5/MESSy2 Atmospheric Chemistry (EMAC) model. We find that NO𝑥 emissions from lightning most importantly affect ozone chemistry at these altitudes.
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.
Sara M. Defratyka, James L. France, Rebecca E. Fisher, Dave Lowry, Julianne M. Fernandez, Semra Bakkaloglu, Camille Yver-Kwok, Jean-Daniel Paris, Philippe Bousquet, Tim Arnold, Chris Rennick, Jon Helmore, Nigel Yarrow, and Euan G. Nisbet
EGUsphere, https://doi.org/10.5194/egusphere-2023-1490, https://doi.org/10.5194/egusphere-2023-1490, 2023
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We are focused on verification of δ13CH4 measurements in near-source conditions and we have provided an insight into the impact of chosen calculation methods for determined isotopic signatures. Our study offers a step forward for establishing an unified, robust, and reliable analytical technique to determine δ13CH4 of methane sources. Our recommended analytical approach reduces biases and uncertainties coming from measurement conditions, data clustering and various available fitting methods.
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.
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.
Seyed Omid Nabavi, Theodoros Christoudias, Yiannis Proestos, Christos Fountoukis, Huda Al-Sulaiti, and Jos Lelieveld
Atmos. Chem. Phys., 23, 7719–7739, https://doi.org/10.5194/acp-23-7719-2023, https://doi.org/10.5194/acp-23-7719-2023, 2023
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The objective of our study is to comprehensively assess the timing of radioactive material transportation and deposition, along with the associated population exposure in the designated region. We employed diverse meteorological inputs, emission specifics, and simulation codes, aiming to quantify the level of uncertainty.
Sophie Wittig, Antoine Berchet, Isabelle Pison, Marielle Saunois, Joël Thanwerdas, Adrien Martinez, Jean-Daniel Paris, Toshinobu Machida, Motoki Sasakawa, Douglas E. J. Worthy, Xin Lan, Rona L. Thompson, Espen Sollum, and Mikhail Arshinov
Atmos. Chem. Phys., 23, 6457–6485, https://doi.org/10.5194/acp-23-6457-2023, https://doi.org/10.5194/acp-23-6457-2023, 2023
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Here, an inverse modelling approach is applied to estimate CH4 sources and sinks in the Arctic from 2008 to 2019. We study the magnitude, seasonal patterns and trends from different sources during recent years. We also assess how the current observation network helps to constrain fluxes. We find that constraints are only significant for North America and, to a lesser extent, West Siberia, where the observation network is relatively dense. We find no clear trend over the period of inversion.
Klaus Klingmüller and Jos Lelieveld
Geosci. Model Dev., 16, 3013–3028, https://doi.org/10.5194/gmd-16-3013-2023, https://doi.org/10.5194/gmd-16-3013-2023, 2023
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Desert dust has significant impacts on climate, public health, infrastructure and ecosystems. An impact assessment requires numerical predictions, which are challenging because the dust emissions are not well known. We present a novel approach using satellite observations and machine learning to more accurately estimate the emissions and to improve the model simulations.
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.
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.
Lisa Ernle, Monika Akima Ringsdorf, and Jonathan Williams
Atmos. Meas. Tech., 16, 1179–1194, https://doi.org/10.5194/amt-16-1179-2023, https://doi.org/10.5194/amt-16-1179-2023, 2023
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Atmospheric ozone can induce artefacts in volatile organic compound measurements. Laboratory tests were made using GC-MS and PTR-MS aircraft systems under tropospheric and stratospheric conditions of humidity and ozone, with and without sodium thiosulfate filter scrubbers. Ozone in dry air produces some carbonyls and degrades alkenes. The scrubber lifetime depends on ozone concentration, flow rate and humidity. For the troposphere with scrubber, no significant artefacts were found over 14 d.
Lenard L. Röder, Patrick Dewald, Clara M. Nussbaumer, Jan Schuladen, John N. Crowley, Jos Lelieveld, and Horst Fischer
Atmos. Meas. Tech., 16, 1167–1178, https://doi.org/10.5194/amt-16-1167-2023, https://doi.org/10.5194/amt-16-1167-2023, 2023
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Field experiments in atmospheric chemistry provide insights into chemical interactions of our atmosphere. However, high data coverage and accuracy are needed to enable further analysis. In this study, we explore a statistical method that combines knowledge about the chemical reactions with information from measurements to increase the quality of field experiment datasets. We test the algorithm for several applications and discuss limitations that depend on the specific variable and the dynamics.
Clément Narbaud, Jean-Daniel Paris, Sophie Wittig, Antoine Berchet, Marielle Saunois, Philippe Nédélec, Boris D. Belan, Mikhail Y. Arshinov, Sergei B. Belan, Denis Davydov, Alexander Fofonov, and Artem Kozlov
Atmos. Chem. Phys., 23, 2293–2314, https://doi.org/10.5194/acp-23-2293-2023, https://doi.org/10.5194/acp-23-2293-2023, 2023
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We measured CH4 and CO2 from aircraft over the Russian Arctic. Analyzing our data with the Lagrangian model FLEXPART, we find a sharp east–west gradient in atmospheric composition. Western Siberia is influenced by strong wetland CH4 emissions, deep CO2 gradient from biospheric uptake, and long-range transport from Europe and North America. Eastern flights document less variability. Over the Arctic Ocean, we find a small influence from marine CH4 emissions compatible with reasonable inventories.
Ryan Vella, Matthew Forrest, Jos Lelieveld, and Holger Tost
Geosci. Model Dev., 16, 885–906, https://doi.org/10.5194/gmd-16-885-2023, https://doi.org/10.5194/gmd-16-885-2023, 2023
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Biogenic volatile organic compounds (BVOCs) are released by vegetation and have a major impact on atmospheric chemistry and aerosol formation. Non-interacting vegetation constrains the majority of numerical models used to estimate global BVOC emissions, and thus, the effects of changing vegetation on emissions are not addressed. In this work, we replace the offline vegetation with dynamic vegetation states by linking a chemistry–climate model with a global dynamic vegetation model.
Jennifer Schallock, Christoph Brühl, Christine Bingen, Michael Höpfner, Landon Rieger, and Jos Lelieveld
Atmos. Chem. Phys., 23, 1169–1207, https://doi.org/10.5194/acp-23-1169-2023, https://doi.org/10.5194/acp-23-1169-2023, 2023
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We characterized the influence of volcanic aerosols for the period 1990–2019 and established a volcanic SO2 emission inventory that includes more than 500 eruptions. From limb-based satellite observations of SO2 and extinction, we derive 3D plumes of SO2 perturbations and injected mass by a novel method. We calculate instantaneous radiative forcing with a comprehensive chemisty climate model. Our results show that smaller eruptions can also contribute to the stratospheric aerosol forcing.
Denis Leppla, Nora Zannoni, Leslie Kremper, Jonathan Williams, Christopher Pöhlker, Marta Sá, Maria Christina Solci, and Thorsten Hoffmann
Atmos. Chem. Phys., 23, 809–820, https://doi.org/10.5194/acp-23-809-2023, https://doi.org/10.5194/acp-23-809-2023, 2023
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Chiral chemodiversity plays a critical role in biochemical processes such as insect and plant communication. Here we report on the measurement of chiral-specified secondary organic aerosol in the Amazon rainforest. The results show that the chiral ratio is mainly determined by large-scale emission processes. Characteristic emissions of chiral aerosol precursors from different forest ecosystems can thus provide large-scale information on different biogenic sources via chiral particle analysis.
Mohamed Abdelkader, Georgiy Stenchikov, Andrea Pozzer, Holger Tost, and Jos Lelieveld
Atmos. Chem. Phys., 23, 471–500, https://doi.org/10.5194/acp-23-471-2023, https://doi.org/10.5194/acp-23-471-2023, 2023
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We study the effect of injected volcanic ash, water vapor, and SO2 on the development of the volcanic cloud and the stratospheric aerosol optical depth (AOD). Both are sensitive to the initial injection height and to the aging of the volcanic ash shaped by heterogeneous chemistry coupled with the ozone cycle. The paper explains the large differences in AOD for different injection scenarios, which could improve the estimate of the radiative forcing of volcanic eruptions.
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.
Laura Tomsche, Andreas Marsing, Tina Jurkat-Witschas, Johannes Lucke, Stefan Kaufmann, Katharina Kaiser, Johannes Schneider, Monika Scheibe, Hans Schlager, Lenard Röder, Horst Fischer, Florian Obersteiner, Andreas Zahn, Martin Zöger, Jos Lelieveld, and Christiane Voigt
Atmos. Chem. Phys., 22, 15135–15151, https://doi.org/10.5194/acp-22-15135-2022, https://doi.org/10.5194/acp-22-15135-2022, 2022
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The detection of sulfur compounds in the upper troposphere (UT) and lower stratosphere (LS) is a challenge. In-flight measurements of SO2 and sulfate aerosol were performed during the BLUESKY mission in spring 2020 under exceptional atmospheric conditions. Reduced sinks in the dry UTLS and lower but still significant air traffic influenced the enhanced SO2 in the UT, and aged volcanic plumes enhanced the LS sulfate aerosol impacting the atmospheric radiation budget and global climate.
Charlotte M. Beall, Thomas C. J. Hill, Paul J. DeMott, Tobias Köneman, Michael Pikridas, Frank Drewnick, Hartwig Harder, Christopher Pöhlker, Jos Lelieveld, Bettina Weber, Minas Iakovides, Roman Prokeš, Jean Sciare, Meinrat O. Andreae, M. Dale Stokes, and Kimberly A. Prather
Atmos. Chem. Phys., 22, 12607–12627, https://doi.org/10.5194/acp-22-12607-2022, https://doi.org/10.5194/acp-22-12607-2022, 2022
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Ice-nucleating particles (INPs) are rare aerosols that can trigger ice formation in clouds and affect climate-relevant cloud properties such as phase, reflectivity and lifetime. Dust is the dominant INP source, yet few measurements have been reported near major dust sources. We report INP observations within hundreds of kilometers of the biggest dust source regions globally: the Sahara and the Arabian Peninsula. Results show that at temperatures > −15 °C, INPs are dominated by organics.
Mengze Li, Andrea Pozzer, Jos Lelieveld, and Jonathan Williams
Earth Syst. Sci. Data, 14, 4351–4364, https://doi.org/10.5194/essd-14-4351-2022, https://doi.org/10.5194/essd-14-4351-2022, 2022
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We present a northern hemispheric airborne measurement dataset of atmospheric ethane, propane and methane and temporal trends for the time period 2006–2016 in the upper troposphere and lower stratosphere. The growth rates of ethane, methane, and propane in the upper troposphere are -2.24, 0.33, and -0.78 % yr-1, respectively, and in the lower stratosphere they are -3.27, 0.26, and -4.91 % yr-1, respectively, in 2006–2016.
Therese S. Carter, Colette L. Heald, Jesse H. Kroll, Eric C. Apel, Donald Blake, Matthew Coggon, Achim Edtbauer, Georgios Gkatzelis, Rebecca S. Hornbrook, Jeff Peischl, Eva Y. Pfannerstill, Felix Piel, Nina G. Reijrink, Akima Ringsdorf, Carsten Warneke, Jonathan Williams, Armin Wisthaler, and Lu Xu
Atmos. Chem. Phys., 22, 12093–12111, https://doi.org/10.5194/acp-22-12093-2022, https://doi.org/10.5194/acp-22-12093-2022, 2022
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Fires emit many gases which can contribute to smog and air pollution. However, the amount and properties of these chemicals are not well understood, so this work updates and expands their representation in a global atmospheric model, including by adding new chemicals. We confirm that this updated representation generally matches measurements taken in several fire regions. We then show that fires provide ~15 % of atmospheric reactivity globally and more than 75 % over fire source regions.
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.
Yunsong Liu, Jean-Daniel Paris, Mihalis Vrekoussis, Panayiota Antoniou, Christos Constantinides, Maximilien Desservettaz, Christos Keleshis, Olivier Laurent, Andreas Leonidou, Carole Philippon, Panagiotis Vouterakos, Pierre-Yves Quéhé, Philippe Bousquet, and Jean Sciare
Atmos. Meas. Tech., 15, 4431–4442, https://doi.org/10.5194/amt-15-4431-2022, https://doi.org/10.5194/amt-15-4431-2022, 2022
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This paper details laboratory-based and field developments of a cost-effective and compacted UAV CO2 sensor system to address the challenge of measuring CO2 with sufficient precision and acquisition frequency. We assess its performance extensively through laboratory and field tests and provide a case study in an urban area (Nicosia, Cyprus). We therefore expect that this portable system will be widely used for measuring CO2 emission and distribution in natural or urban environments.
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.
Marco Wietzoreck, Marios Kyprianou, Benjamin A. Musa Bandowe, Siddika Celik, John N. Crowley, Frank Drewnick, Philipp Eger, Nils Friedrich, Minas Iakovides, Petr Kukučka, Jan Kuta, Barbora Nežiková, Petra Pokorná, Petra Přibylová, Roman Prokeš, Roland Rohloff, Ivan Tadic, Sebastian Tauer, Jake Wilson, Hartwig Harder, Jos Lelieveld, Ulrich Pöschl, Euripides G. Stephanou, and Gerhard Lammel
Atmos. Chem. Phys., 22, 8739–8766, https://doi.org/10.5194/acp-22-8739-2022, https://doi.org/10.5194/acp-22-8739-2022, 2022
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A unique dataset of concentrations and sources of polycyclic aromatic hydrocarbons (PAHs) and their alkylated, oxygenated and nitrated derivatives, in total 74 individual species, in the marine atmosphere is presented. Exposure to these substances poses a major health risk. We found very low concentrations over the Arabian Sea, while both local and long-range-transported pollution caused elevated levels over the Mediterranean Sea and the Arabian Gulf.
Ovid O. Krüger, Bruna A. Holanda, Sourangsu Chowdhury, Andrea Pozzer, David Walter, Christopher Pöhlker, Maria Dolores Andrés Hernández, John P. Burrows, Christiane Voigt, Jos Lelieveld, Johannes Quaas, Ulrich Pöschl, and Mira L. Pöhlker
Atmos. Chem. Phys., 22, 8683–8699, https://doi.org/10.5194/acp-22-8683-2022, https://doi.org/10.5194/acp-22-8683-2022, 2022
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The abrupt reduction in human activities during the first COVID-19 lockdown created unprecedented atmospheric conditions. We took the opportunity to quantify changes in black carbon (BC) as a major anthropogenic air pollutant. Therefore, we measured BC on board a research aircraft over Europe during the lockdown and compared the results to measurements from 2017. With model simulations we account for different weather conditions and find a lockdown-related decrease in BC of 41 %.
Boris D. Belan, Gerard Ancellet, Irina S. Andreeva, Pavel N. Antokhin, Viktoria G. Arshinova, Mikhail Y. Arshinov, Yurii S. Balin, Vladimir E. Barsuk, Sergei B. Belan, Dmitry G. Chernov, Denis K. Davydov, Alexander V. Fofonov, Georgii A. Ivlev, Sergei N. Kotel'nikov, Alexander S. Kozlov, Artem V. Kozlov, Katharine Law, Andrey V. Mikhal'chishin, Igor A. Moseikin, Sergei V. Nasonov, Philippe Nédélec, Olesya V. Okhlopkova, Sergei E. Ol'kin, Mikhail V. Panchenko, Jean-Daniel Paris, Iogannes E. Penner, Igor V. Ptashnik, Tatyana M. Rasskazchikova, Irina K. Reznikova, Oleg A. Romanovskii, Alexander S. Safatov, Denis E. Savkin, Denis V. Simonenkov, Tatyana K. Sklyadneva, Gennadii N. Tolmachev, Semyon V. Yakovlev, and Polina N. Zenkova
Atmos. Meas. Tech., 15, 3941–3967, https://doi.org/10.5194/amt-15-3941-2022, https://doi.org/10.5194/amt-15-3941-2022, 2022
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The change of the global climate is most pronounced in the Arctic, where the air temperature increases faster than the global average. This is associated with an increase in the concentration of greenhouse gases in the atmosphere. It is important to study how the air composition in the Arctic changes in the changing climate. Thus this integrated experiment was carried out to measure the composition of the troposphere in the Russian sector of the Arctic from on board the aircraft laboratory.
Patrick Dewald, Clara M. Nussbaumer, Jan Schuladen, Akima Ringsdorf, Achim Edtbauer, Horst Fischer, Jonathan Williams, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 22, 7051–7069, https://doi.org/10.5194/acp-22-7051-2022, https://doi.org/10.5194/acp-22-7051-2022, 2022
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We measured the gas-phase reactivity of the NO3 radical on the summit (825 m a.s.l.) of a semi-rural mountain in southwestern Germany in July 2021. The impact of VOC-induced NO3 losses (mostly monoterpenes) competing with a loss by reaction with NO and photolysis throughout the diel cycle was estimated. Besides chemistry, boundary layer dynamics and plant-physiological processes presumably have a great impact on our observations, which were compared to previous NO3 measurements at the same site.
George K. Georgiou, Theodoros Christoudias, Yiannis Proestos, Jonilda Kushta, Michael Pikridas, Jean Sciare, Chrysanthos Savvides, and Jos Lelieveld
Geosci. Model Dev., 15, 4129–4146, https://doi.org/10.5194/gmd-15-4129-2022, https://doi.org/10.5194/gmd-15-4129-2022, 2022
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We evaluate the skill of the WRF-Chem model to perform high-resolution air quality forecasts (including ozone, nitrogen dioxide, and fine particulate matter) over the Eastern Mediterranean, during winter and summer. We compare the forecast output to observational data from background and urban locations and the forecast output from CAMS. WRF-Chem was found to forecast the concentrations and diurnal profiles of gas-phase pollutants in urban areas with higher accuracy.
Clara M. Nussbaumer, Andrea Pozzer, Ivan Tadic, Lenard Röder, Florian Obersteiner, Hartwig Harder, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 22, 6151–6165, https://doi.org/10.5194/acp-22-6151-2022, https://doi.org/10.5194/acp-22-6151-2022, 2022
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The European COVID-19 lockdowns have significantly reduced the emission of primary pollutants such as NOx, which impacts the tropospheric photochemical processes and the abundance of O3. In this study, we present how the lockdowns have affected tropospheric trace gases and ozone production based on in situ observations and modeling simulations. We additionally show that the chemical regime shifted from a transition point to a NOx limitation in the upper troposphere.
Wenyu Sun, Matias Berasategui, Andrea Pozzer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 22, 4969–4984, https://doi.org/10.5194/acp-22-4969-2022, https://doi.org/10.5194/acp-22-4969-2022, 2022
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The reaction between OH and SO2 is a termolecular process that in the atmosphere results in the formation of H2SO4 and thus aerosols. We present the first temperature- and pressure-dependent measurements of the rate coefficients in N2. This is also the first study to examine the effects of water vapour on the kinetics of this reaction. Our results indicate the rate coefficient is larger than that recommended by evaluation panels, with deviations of up to 30 % in some parts of the atmosphere.
Hanna K. Lappalainen, Tuukka Petäjä, Timo Vihma, Jouni Räisänen, Alexander Baklanov, Sergey Chalov, Igor Esau, Ekaterina Ezhova, Matti Leppäranta, Dmitry Pozdnyakov, Jukka Pumpanen, Meinrat O. Andreae, Mikhail Arshinov, Eija Asmi, Jianhui Bai, Igor Bashmachnikov, Boris Belan, Federico Bianchi, Boris Biskaborn, Michael Boy, Jaana Bäck, Bin Cheng, Natalia Chubarova, Jonathan Duplissy, Egor Dyukarev, Konstantinos Eleftheriadis, Martin Forsius, Martin Heimann, Sirkku Juhola, Vladimir Konovalov, Igor Konovalov, Pavel Konstantinov, Kajar Köster, Elena Lapshina, Anna Lintunen, Alexander Mahura, Risto Makkonen, Svetlana Malkhazova, Ivan Mammarella, Stefano Mammola, Stephany Buenrostro Mazon, Outi Meinander, Eugene Mikhailov, Victoria Miles, Stanislav Myslenkov, Dmitry Orlov, Jean-Daniel Paris, Roberta Pirazzini, Olga Popovicheva, Jouni Pulliainen, Kimmo Rautiainen, Torsten Sachs, Vladimir Shevchenko, Andrey Skorokhod, Andreas Stohl, Elli Suhonen, Erik S. Thomson, Marina Tsidilina, Veli-Pekka Tynkkynen, Petteri Uotila, Aki Virkkula, Nadezhda Voropay, Tobias Wolf, Sayaka Yasunaka, Jiahua Zhang, Yubao Qiu, Aijun Ding, Huadong Guo, Valery Bondur, Nikolay Kasimov, Sergej Zilitinkevich, Veli-Matti Kerminen, and Markku Kulmala
Atmos. Chem. Phys., 22, 4413–4469, https://doi.org/10.5194/acp-22-4413-2022, https://doi.org/10.5194/acp-22-4413-2022, 2022
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We summarize results during the last 5 years in the northern Eurasian region, especially from Russia, and introduce recent observations of the air quality in the urban environments in China. Although the scientific knowledge in these regions has increased, there are still gaps in our understanding of large-scale climate–Earth surface interactions and feedbacks. This arises from limitations in research infrastructures and integrative data analyses, hindering a comprehensive system analysis.
Yanan Zhao, Dennis Booge, Christa A. Marandino, Cathleen Schlundt, Astrid Bracher, Elliot L. Atlas, Jonathan Williams, and Hermann W. Bange
Biogeosciences, 19, 701–714, https://doi.org/10.5194/bg-19-701-2022, https://doi.org/10.5194/bg-19-701-2022, 2022
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We present here, for the first time, simultaneously measured dimethylsulfide (DMS) seawater concentrations and DMS atmospheric mole fractions from the Peruvian upwelling region during two cruises in December 2012 and October 2015. Our results indicate low oceanic DMS concentrations and atmospheric DMS molar fractions in surface waters and the atmosphere, respectively. In addition, the Peruvian upwelling region was identified as an insignificant source of DMS emissions during both periods.
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.
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.
Vlassis A. Karydis, Alexandra P. Tsimpidi, Andrea Pozzer, and Jos Lelieveld
Atmos. Chem. Phys., 21, 14983–15001, https://doi.org/10.5194/acp-21-14983-2021, https://doi.org/10.5194/acp-21-14983-2021, 2021
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Aerosol particle pH is well-buffered by alkaline compounds, notably NH3 and crustal elements. NH3 is found to supply remarkable buffering capacity on a global scale, from the polluted continents to the remote oceans. Potential future changes in agricultural NH3 must be accompanied by strong reductions of SO2 and NOx to avoid particles becoming highly acidic, with implications for human health (aerosol toxicity), ecosystems (acid deposition), clouds, and climate (aerosol hygroscopicity).
Philipp G. Eger, Luc Vereecken, Rolf Sander, Jan Schuladen, Nicolas Sobanski, Horst Fischer, Einar Karu, Jonathan Williams, Ville Vakkari, Tuukka Petäjä, Jos Lelieveld, Andrea Pozzer, and John N. Crowley
Atmos. Chem. Phys., 21, 14333–14349, https://doi.org/10.5194/acp-21-14333-2021, https://doi.org/10.5194/acp-21-14333-2021, 2021
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We determine the impact of pyruvic acid photolysis on the formation of acetaldehyde and peroxy radicals during summer and autumn in the Finnish boreal forest using a data-constrained box model. Our results are dependent on the chosen scenario in which the overall quantum yield and the photolysis products are varied. We highlight that pyruvic acid photolysis can be an important contributor to acetaldehyde and peroxy radical formation in remote, forested regions.
R. Anthony Cox, Markus Ammann, John N. Crowley, Paul T. Griffiths, Hartmut Herrmann, Erik H. Hoffmann, Michael E. Jenkin, V. Faye McNeill, Abdelwahid Mellouki, Christopher J. Penkett, Andreas Tilgner, and Timothy J. Wallington
Atmos. Chem. Phys., 21, 13011–13018, https://doi.org/10.5194/acp-21-13011-2021, https://doi.org/10.5194/acp-21-13011-2021, 2021
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The term open-air factor was coined in the 1960s, establishing that rural air had powerful germicidal properties possibly resulting from immediate products of the reaction of ozone with alkenes, unsaturated compounds ubiquitously present in natural and polluted environments. We have re-evaluated those early experiments, applying the recently substantially improved knowledge, and put them into the context of the lifetime of aerosol-borne pathogens that are so important in the Covid-19 pandemic.
James Weber, Scott Archer-Nicholls, Nathan Luke Abraham, Youngsub M. Shin, Thomas J. Bannan, Carl J. Percival, Asan Bacak, Paulo Artaxo, Michael Jenkin, M. Anwar H. Khan, Dudley E. Shallcross, Rebecca H. Schwantes, Jonathan Williams, and Alex T. Archibald
Geosci. Model Dev., 14, 5239–5268, https://doi.org/10.5194/gmd-14-5239-2021, https://doi.org/10.5194/gmd-14-5239-2021, 2021
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The new mechanism CRI-Strat 2 features state-of-the-art isoprene chemistry not previously available in UKCA and improves UKCA's ability to reproduce observed concentrations of isoprene, monoterpenes, and OH in tropical regions. The enhanced ability to model isoprene, the most widely emitted non-methane volatile organic compound (VOC), will allow understanding of how isoprene and other biogenic VOCs affect atmospheric composition and, through biosphere–atmosphere feedbacks, climate change.
Jean-Daniel Paris, Aurélie Riandet, Efstratios Bourtsoukidis, Marc Delmotte, Antoine Berchet, Jonathan Williams, Lisa Ernle, Ivan Tadic, Hartwig Harder, and Jos Lelieveld
Atmos. Chem. Phys., 21, 12443–12462, https://doi.org/10.5194/acp-21-12443-2021, https://doi.org/10.5194/acp-21-12443-2021, 2021
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We measured atmospheric methane and CO2 by ship in the Middle East. We probe the origin of methane with a combination of light alkane measurements and modeling. We find strong influence from nearby oil and gas production over the Arabian Gulf. Comparing our data to inventories indicates that inventories overestimate sources from the upstream gas industry but underestimate emissions from oil extraction and processing. The Red Sea was under a complex mixture of sources due to human activity.
Patrick Dewald, Raphael Dörich, Jan Schuladen, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 14, 5501–5519, https://doi.org/10.5194/amt-14-5501-2021, https://doi.org/10.5194/amt-14-5501-2021, 2021
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Organic nitrates generated from the reaction between isoprene and the nitrate radical (ISOP-NITs) were detected via their thermal dissociation in heated quartz inlets to nitrogen dioxide monitored by cavity ring-down spectroscopy. The temperature-dependent dissociation profiles of ISOP-NITs in the presence of ozone (O3) are broad in contrast to narrow profiles of common reference compounds. We demonstrate that this broadening is caused by O3-assisted reactions of ISOP-NITs on quartz surfaces.
Raphael Dörich, Philipp Eger, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 14, 5319–5332, https://doi.org/10.5194/amt-14-5319-2021, https://doi.org/10.5194/amt-14-5319-2021, 2021
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We demonstrate in laboratory experiments that the formation of IOx anions (formed in reactions of I− with O3) or acetate anions (formed e.g. by the reaction of I− with peracetic acid) results in unexpected sensitivity of an iodide chemical ionisation mass spectrometer (I-CIMS) to HNO3 at a mass-to-charge ratio of 62. This helps explain observations of apparent high daytime levels of N2O5. Airborne measurements using I-CIMS confirm these conclusions.
Vinod Kumar, Julia Remmers, Steffen Beirle, Joachim Fallmann, Astrid Kerkweg, Jos Lelieveld, Mariano Mertens, Andrea Pozzer, Benedikt Steil, Marc Barra, Holger Tost, and Thomas Wagner
Atmos. Meas. Tech., 14, 5241–5269, https://doi.org/10.5194/amt-14-5241-2021, https://doi.org/10.5194/amt-14-5241-2021, 2021
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We present high-resolution regional atmospheric chemistry model simulations focused around Germany. We highlight the importance of spatial resolution of the model itself as well as the input emissions inventory and short-scale temporal variability of emissions for simulations. We propose a consistent approach for evaluating the simulated vertical distribution of NO2 using MAX-DOAS measurements while also considering its spatial sensitivity volume and change in sensitivity within this volume.
Sara M. Defratyka, Jean-Daniel Paris, Camille Yver-Kwok, Daniel Loeb, James France, Jon Helmore, Nigel Yarrow, Valérie Gros, and Philippe Bousquet
Atmos. Meas. Tech., 14, 5049–5069, https://doi.org/10.5194/amt-14-5049-2021, https://doi.org/10.5194/amt-14-5049-2021, 2021
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We consider the possibility of using the CRDS Picarro G2201-i instrument, originally designed for isotopic CH4 and CO2, for measurements of ethane : methane in near-source conditions. The work involved laboratory tests, a controlled release experiment and mobile measurements. We show the potential of determining ethane : methane with 50 ppb ethane uncertainty. The instrument can correctly estimate the ratio in CH4 enhancements of 1 ppm and more, as can be found at strongly emitting sites.
Klaus Klingmüller and Jos Lelieveld
Geosci. Model Dev., 14, 4429–4441, https://doi.org/10.5194/gmd-14-4429-2021, https://doi.org/10.5194/gmd-14-4429-2021, 2021
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Soil moisture is of great importance for weather and climate. We present a machine learning model that produces accurate predictions of satellite-observed surface soil moisture, based on meteorological data from a climate model. It can be used as soil moisture parametrisation in climate models and to produce comprehensive global soil moisture datasets. Moreover, it may motivate similar applications of machine learning in climate science.
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.
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.
Clara M. Nussbaumer, Ivan Tadic, Dirk Dienhart, Nijing Wang, Achim Edtbauer, Lisa Ernle, Jonathan Williams, Florian Obersteiner, Isidoro Gutiérrez-Álvarez, Hartwig Harder, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 7933–7945, https://doi.org/10.5194/acp-21-7933-2021, https://doi.org/10.5194/acp-21-7933-2021, 2021
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Lightning over continental and coastal areas is frequent and accompanied by deep convection, while lightning over marine areas and particularly in tropical cyclones is rare. This research presents in situ observations of the tropical storm Florence 2018 near Cabo Verde. We show the absence of lightning in the tropical storm despite the occurrence of deep convective processes by atmospheric trace gas measurements of O3, NO, CO, H2O2, DMS and CH2I.
Nils Friedrich, Philipp Eger, Justin Shenolikar, Nicolas Sobanski, Jan Schuladen, Dirk Dienhart, Bettina Hottmann, Ivan Tadic, Horst Fischer, Monica Martinez, Roland Rohloff, Sebastian Tauer, Hartwig Harder, Eva Y. Pfannerstill, Nijing Wang, Jonathan Williams, James Brooks, Frank Drewnick, Hang Su, Guo Li, Yafang Cheng, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 21, 7473–7498, https://doi.org/10.5194/acp-21-7473-2021, https://doi.org/10.5194/acp-21-7473-2021, 2021
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This paper uses NOx and NOz measurements from the 2017 AQABA ship campaign in the Mediterranean Sea and around the Arabian Peninsula to examine the influence e.g. of emissions from shipping and oil and gas production. Night-time losses of NOx dominated in the Arabian Gulf and in the Red Sea, whereas daytime losses were more important in the Mediterranean Sea. Nitric acid and organic nitrates were the most prevalent components of NOz.
Eva Y. Pfannerstill, Nina G. Reijrink, Achim Edtbauer, Akima Ringsdorf, Nora Zannoni, Alessandro Araújo, Florian Ditas, Bruna A. Holanda, Marta O. Sá, Anywhere Tsokankunku, David Walter, Stefan Wolff, Jošt V. Lavrič, Christopher Pöhlker, Matthias Sörgel, and Jonathan Williams
Atmos. Chem. Phys., 21, 6231–6256, https://doi.org/10.5194/acp-21-6231-2021, https://doi.org/10.5194/acp-21-6231-2021, 2021
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Tropical forests are globally significant for atmospheric chemistry. However, the mixture of reactive organic gases emitted by these ecosystems is poorly understood. By comprehensive observations at an Amazon forest site, we show that oxygenated species were previously underestimated in their contribution to the tropical-forest reactant mix. Our results show rain and temperature effects and have implications for models and the understanding of ozone and particle formation above tropical forests.
Abdelwahid Mellouki, Markus Ammann, R. Anthony Cox, John N. Crowley, Hartmut Herrmann, Michael E. Jenkin, V. Faye McNeill, Jürgen Troe, and Timothy J. Wallington
Atmos. Chem. Phys., 21, 4797–4808, https://doi.org/10.5194/acp-21-4797-2021, https://doi.org/10.5194/acp-21-4797-2021, 2021
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Volatile organic compounds play an important role in atmospheric chemistry. This article, the eighth in the series, presents kinetic and photochemical data sheets evaluated by the IUPAC Task Group on Atmospheric Chemical Kinetic Data Evaluation. It covers the gas-phase reactions of organic species with four, or more, carbon atoms (≥ C4) including thermal reactions of closed-shell organic species with HO and NO3 radicals and their photolysis. These data are important for atmospheric models.
Wenjie Wang, Jipeng Qi, Jun Zhou, Bin Yuan, Yuwen Peng, Sihang Wang, Suxia Yang, Jonathan Williams, Vinayak Sinha, and Min Shao
Atmos. Meas. Tech., 14, 2285–2298, https://doi.org/10.5194/amt-14-2285-2021, https://doi.org/10.5194/amt-14-2285-2021, 2021
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We designed a new reactor for measurements of OH reactivity (i.e., OH radical loss frequency) based on the comparative reactivity method under
high-NOx conditions, such as in cities. We performed a series of laboratory tests to evaluate the new reactor. The new reactor was used in the field and performed well in measuring OH reactivity in air influenced by upwind cities.
Einar Karu, Mengze Li, Lisa Ernle, Carl A. M. Brenninkmeijer, Jos Lelieveld, and Jonathan Williams
Atmos. Meas. Tech., 14, 1817–1831, https://doi.org/10.5194/amt-14-1817-2021, https://doi.org/10.5194/amt-14-1817-2021, 2021
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A gas measurement device was developed to measure trace gases (ppt level) in the air based on an atomic emission detector. It combines a cryogenic pre-concentrator (CryoTrap), a gas chromatograph (GC), and a new high-resolution atomic emission detector (AED). The CryoTrap–GC–AED instrumental setup, limits of detection, and elemental performance are presented and discussed. Two measurement case studies are reported: one in a Finnish boreal forest and the other based on an aircraft campaign.
Domenico Taraborrelli, David Cabrera-Perez, Sara Bacer, Sergey Gromov, Jos Lelieveld, Rolf Sander, and Andrea Pozzer
Atmos. Chem. Phys., 21, 2615–2636, https://doi.org/10.5194/acp-21-2615-2021, https://doi.org/10.5194/acp-21-2615-2021, 2021
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Atmospheric pollutants from anthropogenic activities and biomass burning are usually regarded as ozone precursors. Monocyclic aromatics are no exception. Calculations with a comprehensive atmospheric model are consistent with this view but only for air masses close to pollution source regions. However, the same model predicts that aromatics, when transported to remote areas, may effectively destroy ozone. This loss of tropospheric ozone rivals the one attributed to bromine.
Sara Bacer, Sylvia C. Sullivan, Odran Sourdeval, Holger Tost, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 21, 1485–1505, https://doi.org/10.5194/acp-21-1485-2021, https://doi.org/10.5194/acp-21-1485-2021, 2021
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We investigate the relative importance of the rates of both microphysical processes and unphysical correction terms that act as sources or sinks of ice crystals in cold clouds. By means of numerical simulations performed with a global chemistry–climate model, we assess the relevance of these rates at global and regional scales. This estimation is of fundamental importance to assign priority to the development of microphysics parameterizations and compare model output with observations.
Klaus Klingmüller, Vlassis A. Karydis, Sara Bacer, Georgiy L. Stenchikov, and Jos Lelieveld
Atmos. Chem. Phys., 20, 15285–15295, https://doi.org/10.5194/acp-20-15285-2020, https://doi.org/10.5194/acp-20-15285-2020, 2020
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Particulate air pollution cools the climate and partially masks the greenhouse warming by reflecting sunlight and enhancing the reflection by clouds. The intensity of this cooling depends on interactions between pollution and desert dust within the atmosphere. Our simulations with a global atmospheric chemistry-climate model indicate that these interactions significantly weaken the cooling.
Matias Berasategui, Damien Amedro, Luc Vereecken, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 13541–13555, https://doi.org/10.5194/acp-20-13541-2020, https://doi.org/10.5194/acp-20-13541-2020, 2020
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Peracetic acid is one of the most abundant organic peroxides in the atmosphere. We combine experiments and theory to show that peracetic acid reacts orders of magnitude more slowly with OH than presently accepted, which results in a significant extension of its atmospheric lifetime.
R. Anthony Cox, Markus Ammann, John N. Crowley, Hartmut Herrmann, Michael E. Jenkin, V. Faye McNeill, Abdelwahid Mellouki, Jürgen Troe, and Timothy J. Wallington
Atmos. Chem. Phys., 20, 13497–13519, https://doi.org/10.5194/acp-20-13497-2020, https://doi.org/10.5194/acp-20-13497-2020, 2020
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Criegee intermediates, formed from alkene–ozone reactions, play a potentially important role as tropospheric oxidants. Evaluated kinetic data are provided for reactions governing their formation and removal for use in atmospheric models. These include their formation from reactions of simple and complex alkenes and removal by decomposition and reaction with a number of atmospheric species (e.g. H2O, SO2). An overview of the tropospheric chemistry of Criegee intermediates is also provided.
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.
Nils Friedrich, Ivan Tadic, Jan Schuladen, James Brooks, Eoghan Darbyshire, Frank Drewnick, Horst Fischer, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 13, 5739–5761, https://doi.org/10.5194/amt-13-5739-2020, https://doi.org/10.5194/amt-13-5739-2020, 2020
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We present a new instrument for the measurement of NOx and NOy based on a combination of the thermal dissociation of NOy to NOx and cavity ring-down spectroscopic detection of NO2. It features a denuder to separate the contributions of gas-phase and particulate nitrates to NOy. We provide a detailed characterization of the instrument and briefly outline results from first deployments.
Nijing Wang, Achim Edtbauer, Christof Stönner, Andrea Pozzer, Efstratios Bourtsoukidis, Lisa Ernle, Dirk Dienhart, Bettina Hottmann, Horst Fischer, Jan Schuladen, John N. Crowley, Jean-Daniel Paris, Jos Lelieveld, and Jonathan Williams
Atmos. Chem. Phys., 20, 10807–10829, https://doi.org/10.5194/acp-20-10807-2020, https://doi.org/10.5194/acp-20-10807-2020, 2020
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Carbonyl compounds were measured on a ship travelling around the Arabian Peninsula in summer 2017, crossing both highly polluted and extremely clean regions of the marine boundary layer. We investigated the sources and sinks of carbonyls. The results from a global model showed a significant model underestimation for acetaldehyde, a molecule that can influence regional air chemistry. By adding a diurnal oceanic source, the model estimation was highly improved.
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.
Tuukka Petäjä, Ella-Maria Duplissy, Ksenia Tabakova, Julia Schmale, Barbara Altstädter, Gerard Ancellet, Mikhail Arshinov, Yurii Balin, Urs Baltensperger, Jens Bange, Alison Beamish, Boris Belan, Antoine Berchet, Rossana Bossi, Warren R. L. Cairns, Ralf Ebinghaus, Imad El Haddad, Beatriz Ferreira-Araujo, Anna Franck, Lin Huang, Antti Hyvärinen, Angelika Humbert, Athina-Cerise Kalogridis, Pavel Konstantinov, Astrid Lampert, Matthew MacLeod, Olivier Magand, Alexander Mahura, Louis Marelle, Vladimir Masloboev, Dmitri Moisseev, Vaios Moschos, Niklas Neckel, Tatsuo Onishi, Stefan Osterwalder, Aino Ovaska, Pauli Paasonen, Mikhail Panchenko, Fidel Pankratov, Jakob B. Pernov, Andreas Platis, Olga Popovicheva, Jean-Christophe Raut, Aurélie Riandet, Torsten Sachs, Rosamaria Salvatori, Roberto Salzano, Ludwig Schröder, Martin Schön, Vladimir Shevchenko, Henrik Skov, Jeroen E. Sonke, Andrea Spolaor, Vasileios K. Stathopoulos, Mikko Strahlendorff, Jennie L. Thomas, Vito Vitale, Sterios Vratolis, Carlo Barbante, Sabine Chabrillat, Aurélien Dommergue, Konstantinos Eleftheriadis, Jyri Heilimo, Kathy S. Law, Andreas Massling, Steffen M. Noe, Jean-Daniel Paris, André S. H. Prévôt, Ilona Riipinen, Birgit Wehner, Zhiyong Xie, and Hanna K. Lappalainen
Atmos. Chem. Phys., 20, 8551–8592, https://doi.org/10.5194/acp-20-8551-2020, https://doi.org/10.5194/acp-20-8551-2020, 2020
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The role of polar regions is increasing in terms of megatrends such as globalization, new transport routes, demography, and the use of natural resources with consequent effects on regional and transported pollutant concentrations. Here we summarize initial results from our integrative project exploring the Arctic environment and pollution to deliver data products, metrics, and indicators for stakeholders.
Dominik Stolzenburg, Mario Simon, Ananth Ranjithkumar, Andreas Kürten, Katrianne Lehtipalo, Hamish Gordon, Sebastian Ehrhart, Henning Finkenzeller, Lukas Pichelstorfer, Tuomo Nieminen, Xu-Cheng He, Sophia Brilke, Mao Xiao, António Amorim, Rima Baalbaki, Andrea Baccarini, Lisa Beck, Steffen Bräkling, Lucía Caudillo Murillo, Dexian Chen, Biwu Chu, Lubna Dada, António Dias, Josef Dommen, Jonathan Duplissy, Imad El Haddad, Lukas Fischer, Loic Gonzalez Carracedo, Martin Heinritzi, Changhyuk Kim, Theodore K. Koenig, Weimeng Kong, Houssni Lamkaddam, Chuan Ping Lee, Markus Leiminger, Zijun Li, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Tatjana Müller, Wei Nie, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Matti P. Rissanen, Birte Rörup, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Mingyi Wang, Yonghong Wang, Stefan K. Weber, Daniela Wimmer, Peter J. Wlasits, Yusheng Wu, Qing Ye, Marcel Zauner-Wieczorek, Urs Baltensperger, Kenneth S. Carslaw, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Armin Hansel, Markku Kulmala, Jos Lelieveld, Rainer Volkamer, Jasper Kirkby, and Paul M. Winkler
Atmos. Chem. Phys., 20, 7359–7372, https://doi.org/10.5194/acp-20-7359-2020, https://doi.org/10.5194/acp-20-7359-2020, 2020
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Sulfuric acid is a major atmospheric vapour for aerosol formation. If new particles grow fast enough, they can act as cloud droplet seeds or affect air quality. In a controlled laboratory set-up, we demonstrate that van der Waals forces enhance growth from sulfuric acid. We disentangle the effects of ammonia, ions and particle hydration, presenting a complete picture of sulfuric acid growth from molecular clusters onwards. In a climate model, we show its influence on the global aerosol budget.
Ivan Tadic, John N. Crowley, Dirk Dienhart, Philipp Eger, Hartwig Harder, Bettina Hottmann, Monica Martinez, Uwe Parchatka, Jean-Daniel Paris, Andrea Pozzer, Roland Rohloff, Jan Schuladen, Justin Shenolikar, Sebastian Tauer, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 20, 6769–6787, https://doi.org/10.5194/acp-20-6769-2020, https://doi.org/10.5194/acp-20-6769-2020, 2020
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We present shipborne observations of NO, NO2, O3, HCHO, OH, HO2, H2O and the actinic flux obtained in the marine boundary layer (MBL) around the Arabian Peninsula during the summer 2017 AQABA ship campaign. NOx (NO+NO2) and O3 observations clearly showed anthropogenic influence in the MBL around the Arabian Peninsula. The observations were also used to calculate net O3 production in the MBL around the Arabian Peninsula, which was greatest over the northern Red Sea, Oman Gulf and Arabian Gulf.
Daniel Marno, Cheryl Ernest, Korbinian Hens, Umar Javed, Thomas Klimach, Monica Martinez, Markus Rudolf, Jos Lelieveld, and Hartwig Harder
Atmos. Meas. Tech., 13, 2711–2731, https://doi.org/10.5194/amt-13-2711-2020, https://doi.org/10.5194/amt-13-2711-2020, 2020
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In this study, a calibration device for OH and HO2 instruments is characterized at pressures of 275 to 1000 mbar, allowing instrument pressure sensitivity to be quantified to an accuracy of 22 % (1σ). Computational fluid dynamic simulations supporting the understanding of interactions between generated HOx and the instrument inlet led to enhanced determination of factors affecting instrument sensitivity.
Achim Edtbauer, Christof Stönner, Eva Y. Pfannerstill, Matias Berasategui, David Walter, John N. Crowley, Jos Lelieveld, and Jonathan Williams
Atmos. Chem. Phys., 20, 6081–6094, https://doi.org/10.5194/acp-20-6081-2020, https://doi.org/10.5194/acp-20-6081-2020, 2020
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Marine regions where deep nutrient-rich water is pushed towards the surface are called upwelling regions. In these nutrient-rich waters large algal blooms form which are the basis of the marine food web. We measured methane sulfonamide, a molecule containing sulfur and nitrogen, for the first time in ambient air and could show that the origin of this emission is an algal bloom near the Somalia upwelling. Sulfur-containing compounds from algae can promote particle formation over the oceans.
Peter H. Zimmermann, Carl A. M. Brenninkmeijer, Andrea Pozzer, Patrick Jöckel, Franziska Winterstein, Andreas Zahn, Sander Houweling, and Jos Lelieveld
Atmos. Chem. Phys., 20, 5787–5809, https://doi.org/10.5194/acp-20-5787-2020, https://doi.org/10.5194/acp-20-5787-2020, 2020
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The atmospheric abundance of the greenhouse gas methane is determined by interacting emission sources and sinks in a dynamic global environment. In this study, its global budget from 1997 to 2016 is simulated with a general circulation model using emission estimates of 11 source categories. The model results are evaluated against 17 ground station and 320 intercontinental flight observation series. Deviations are used to re-scale the emission quantities with the aim of matching observations.
Siddika Celik, Frank Drewnick, Friederike Fachinger, James Brooks, Eoghan Darbyshire, Hugh Coe, Jean-Daniel Paris, Philipp G. Eger, Jan Schuladen, Ivan Tadic, Nils Friedrich, Dirk Dienhart, Bettina Hottmann, Horst Fischer, John N. Crowley, Hartwig Harder, and Stephan Borrmann
Atmos. Chem. Phys., 20, 4713–4734, https://doi.org/10.5194/acp-20-4713-2020, https://doi.org/10.5194/acp-20-4713-2020, 2020
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Analysis of 252 ship emission plumes in the Mediterranean Sea and around the Arabian Peninsula examined particulate- and gas-phase characteristics. By identifying the corresponding ships, source features and plume age were determined. Emission factors (amount of pollutant per kilogram of fuel burned) were calculated and investigated for dependencies on source characteristics, atmospheric conditions, and transport time, providing insight into the most relevant influences on ship emissions.
Antonin Zabukovec, Gerard Ancellet, Iwan E. Penner, Mikhail Arshinov, Valery Kozlov, Jacques Pelon, Jean-Daniel Paris, Grigory Kokhanenko, Yuri S. Balin, Dmitry Chernov, and Boris D. Belan
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-195, https://doi.org/10.5194/acp-2020-195, 2020
Preprint withdrawn
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Description of two aircraft campaigns results carried out over Siberia in 2013 and 2017 to characterize aerosol emission. A methodology is proposed to derive the aerosol types using transport model and satellite observations. The extinction to backscatter ratio for each aerosol types is reported as it is a key parameter to constrain their radiative impact. These results are compared to previous work conducted in other regions and to aerosol data products observed by spaceborne lidars.
Antoine Berchet, Isabelle Pison, Patrick M. Crill, Brett Thornton, Philippe Bousquet, Thibaud Thonat, Thomas Hocking, Joël Thanwerdas, Jean-Daniel Paris, and Marielle Saunois
Atmos. Chem. Phys., 20, 3987–3998, https://doi.org/10.5194/acp-20-3987-2020, https://doi.org/10.5194/acp-20-3987-2020, 2020
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Methane isotopes in the atmosphere can help us differentiate between emission processes. A large variety of natural and anthropogenic emission types are active in the Arctic and are unsatisfactorily understood and documented up to now. A ship-based campaign was carried out in summer 2014, providing a unique dataset of isotopic measurements in the Arctic Ocean. Using a chemistry-transport model, we link these measurements to circumpolar emissions and retrieve information about their signature.
Philipp G. Eger, Jan Schuladen, Nicolas Sobanski, Horst Fischer, Einar Karu, Jonathan Williams, Matthieu Riva, Qiaozhi Zha, Mikael Ehn, Lauriane L. J. Quéléver, Simon Schallhart, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 3697–3711, https://doi.org/10.5194/acp-20-3697-2020, https://doi.org/10.5194/acp-20-3697-2020, 2020
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Pyruvic acid, CH3C(O)C(O)OH, is an organic acid of biogenic origin that plays a crucial role in plant metabolism, is present in tropospheric air in both gas-phase and aerosol-phase, and is implicated in the formation of secondary organic aerosols. From the first gas-phase measurements of pyruvic acid in the Finnish boreal forest in September 2016 we derive its source strength and discuss potential sources and sinks, with a focus on the relevance of gas-phase pyruvic acid for radical chemistry.
Matthew Forrest, Holger Tost, Jos Lelieveld, and Thomas Hickler
Geosci. Model Dev., 13, 1285–1309, https://doi.org/10.5194/gmd-13-1285-2020, https://doi.org/10.5194/gmd-13-1285-2020, 2020
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We have integrated the LPJ-GUESS dynamic global vegetation model into the EMAC atmospheric chemistry-enabled GCM (general circulation model). This combined framework will enable the investigation of many land–atmosphere interactions and feedbacks with state-of-the-art simulation models. Initial results show that using the climate produced by EMAC together with LPJ-GUESS produces an acceptable representation of the global vegetation.
Damien Amedro, Matias Berasategui, Arne J. C. Bunkan, Andrea Pozzer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 3091–3105, https://doi.org/10.5194/acp-20-3091-2020, https://doi.org/10.5194/acp-20-3091-2020, 2020
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Our laboratory experiments show that the rate coefficient for the termolecular reaction between OH and NO2 is enhanced in the presence of water vapour. Using a chemistry transport model we show that our new parameterization of the temperature, pressure, and bath-gas dependence of this reaction has a significant impact on, for example, NOx and the HNO2 / NO2 ratio when compared to present recommendations.
Matias Berasategui, Damien Amedro, Achim Edtbauer, Jonathan Williams, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 2695–2707, https://doi.org/10.5194/acp-20-2695-2020, https://doi.org/10.5194/acp-20-2695-2020, 2020
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We have determined the rate coefficient and mechanism for the reaction of the OH radical with methane sulphonamide, a trace gas which has recently been found in the atmosphere. The rate coefficient is 1.4 × 10−13 cm3 molec.−1 s−1, which indicates a tropospheric lifetime of > 2 months. The observation of CO, CO2, SO2, HNO3, HCOOH, and N2O products enabled us to derive a detailed reaction mechanism for the reaction, which proceeds predominantly by H abstraction from the CH3 group.
Ying Chen, Yafang Cheng, Nan Ma, Chao Wei, Liang Ran, Ralf Wolke, Johannes Größ, Qiaoqiao Wang, Andrea Pozzer, Hugo A. C. Denier van der Gon, Gerald Spindler, Jos Lelieveld, Ina Tegen, Hang Su, and Alfred Wiedensohler
Atmos. Chem. Phys., 20, 771–786, https://doi.org/10.5194/acp-20-771-2020, https://doi.org/10.5194/acp-20-771-2020, 2020
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Particulate nitrate is one of the most important climate cooling agents. Our results show that interaction with sea-salt aerosol can shift nitrate to larger sized particles (redistribution effect), weakening its direct cooling effect. The modelling results indicate strong redistribution over coastal and offshore regions worldwide as well as continental Europe. Improving the consideration of the redistribution effect in global models fosters a better understanding of climate change.
Tanja J. Schuck, Ann-Katrin Blank, Elisa Rittmeier, Jonathan Williams, Carl A. M. Brenninkmeijer, Andreas Engel, and Andreas Zahn
Atmos. Meas. Tech., 13, 73–84, https://doi.org/10.5194/amt-13-73-2020, https://doi.org/10.5194/amt-13-73-2020, 2020
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Air sample collection aboard aircraft is a tool to measure atmospheric trace gas mixing ratios at altitude. We present results on the stability of 28 halocarbons during storage of air samples collected in stainless-steel flasks inside an automated air sampling unit which is part of the CARIBIC instrument package. Selected fluorinated compounds grew during the experiments while short-lived compounds were depleted. Individual substances were additionally influenced by high mixing ratios of ozone.
Philipp G. Eger, Nils Friedrich, Jan Schuladen, Justin Shenolikar, Horst Fischer, Ivan Tadic, Hartwig Harder, Monica Martinez, Roland Rohloff, Sebastian Tauer, Frank Drewnick, Friederike Fachinger, James Brooks, Eoghan Darbyshire, Jean Sciare, Michael Pikridas, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 19, 12121–12140, https://doi.org/10.5194/acp-19-12121-2019, https://doi.org/10.5194/acp-19-12121-2019, 2019
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Shipborne measurements of nitryl chloride (ClNO2) were made during the AQABA (Air Quality and climate change in the Arabian BAsin) ship campaign in summer 2017. The dataset includes measurements over the Mediterranean Sea and around the Arabian Peninsula with observed mixing ratios ranging from the limit of detection to 600 pptv. We examined the regional variability in the generation of ClNO2 and its importance for Cl atom generation in a marine boundary layer influenced by ships and industry.
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.
Matthias Kippenberger, Gerhard Schuster, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 19, 11939–11951, https://doi.org/10.5194/acp-19-11939-2019, https://doi.org/10.5194/acp-19-11939-2019, 2019
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We investigated the uptake of several trace gases to growing ice surfaces at temperatures relevant to cirrus clouds. HCl, a strong inorganic acid that ionises at the surface, was efficiently trapped in the growing ice, whereas oxidised organic trace gases, which attach to ice by hydrogen bonding, were not. HCl can be efficiently and rapidly removed from the gas phase in supersaturated ice clouds.
Michal Lacko, Nijing Wang, Kristýna Sovová, Pavel Pásztor, and Patrik Španěl
Atmos. Meas. Tech., 12, 4965–4982, https://doi.org/10.5194/amt-12-4965-2019, https://doi.org/10.5194/amt-12-4965-2019, 2019
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The soft chemical ionization analytical technique of selected ion flow tube mass spectrometry, SIFT-MS, was enhanced by a fast GC pre-separation unit to identify individual isomers. Experiments were carried out with two GC columns, MXT-1 and MXT-Volatiles, using two reagent ions, H3O+ and NO+, on monoterpene samples (an artificial mixture and coniferous needles). Analyses of product ion ratios allowed for quantification of multiple monoterpenes in partially separated chromatograms.
Jianzhong Ma, Christoph Brühl, Qianshan He, Benedikt Steil, Vlassis A. Karydis, Klaus Klingmüller, Holger Tost, Bin Chen, Yufang Jin, Ningwei Liu, Xiangde Xu, Peng Yan, Xiuji Zhou, Kamal Abdelrahman, Andrea Pozzer, and Jos Lelieveld
Atmos. Chem. Phys., 19, 11587–11612, https://doi.org/10.5194/acp-19-11587-2019, https://doi.org/10.5194/acp-19-11587-2019, 2019
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We find a pronounced maximum in aerosol extinction in the upper troposphere and lower stratosphere over the Tibetan Plateau during the Asian summer monsoon, caused mainly by mineral dust emitted from the northern Tibetan Plateau and slope area, lofted to and accumulating within the anticyclonic circulation. Mineral dust, water-soluble compounds, such as nitrate and sulfate, and associated liquid water dominate aerosol extinction around the tropopause within the Asian summer monsoon anticyclone.
Eva Y. Pfannerstill, Nijing Wang, Achim Edtbauer, Efstratios Bourtsoukidis, John N. Crowley, Dirk Dienhart, Philipp G. Eger, Lisa Ernle, Horst Fischer, Bettina Hottmann, Jean-Daniel Paris, Christof Stönner, Ivan Tadic, David Walter, Jos Lelieveld, and Jonathan Williams
Atmos. Chem. Phys., 19, 11501–11523, https://doi.org/10.5194/acp-19-11501-2019, https://doi.org/10.5194/acp-19-11501-2019, 2019
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The Arabian Peninsula is a global hot spot of ozone pollution. Our measurements, made on a ship in summer 2017, indicate underlying reasons. Despite being at sea, we observed ozone-forming reactive trace gases (measured as so-called total OH reactivity) comparable to highly populated urban regions in amount and composition. This is due to strong emissions from oil extraction and ship traffic. These emissions were quickly converted to ozone due to intense solar irradiation and high temperatures.
Damien Amedro, Arne J. C. Bunkan, Matias Berasategui, and John N. Crowley
Atmos. Chem. Phys., 19, 10643–10657, https://doi.org/10.5194/acp-19-10643-2019, https://doi.org/10.5194/acp-19-10643-2019, 2019
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The reaction between the OH radical and nitrogen dioxide plays a critical role in controlling abundances of HOx and NOx from the boundary layer to the stratosphere. Uncertainties associated with the rate coefficient for this reaction lead to uncertainty in model predictions of the oxidizing capacity of the atmosphere and photochemical ozone production. We present accurate measurements of the rate coefficient over a range of temperatures and pressures.
Jonathan Liebmann, Nicolas Sobanski, Jan Schuladen, Einar Karu, Heidi Hellén, Hannele Hakola, Qiaozhi Zha, Mikael Ehn, Matthieu Riva, Liine Heikkinen, Jonathan Williams, Horst Fischer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 19, 10391–10403, https://doi.org/10.5194/acp-19-10391-2019, https://doi.org/10.5194/acp-19-10391-2019, 2019
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The formation of alkyl nitrates in the boreal forest was dominated by reactions of the NO3 radical with terpenes, both during the day and the night, with fewer contributions from OH and ozone. The alkyl nitrates formed had lifetimes on the order of 2 h, reflecting efficient loss via uptake to aerosol and deposition.
Erin Evoy, Adrian M. Maclean, Grazia Rovelli, Ying Li, Alexandra P. Tsimpidi, Vlassis A. Karydis, Saeid Kamal, Jos Lelieveld, Manabu Shiraiwa, Jonathan P. Reid, and Allan K. Bertram
Atmos. Chem. Phys., 19, 10073–10085, https://doi.org/10.5194/acp-19-10073-2019, https://doi.org/10.5194/acp-19-10073-2019, 2019
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We measured the diffusion rates of organic molecules in a number of proxies for secondary organic aerosol (SOA) and compared measured diffusion with predictions from two relations: the Stokes–Einstein relation and a fractional Stokes–Einstein relation. The fractional relation does a better job of predicting diffusion rates in this case. Output from an atmospheric model shows that mixing times predicted using the two relations differ by up to 1 order of magnitude at an altitude of ~ 3 km.
Jan-Marcus Nasse, Philipp G. Eger, Denis Pöhler, Stefan Schmitt, Udo Frieß, and Ulrich Platt
Atmos. Meas. Tech., 12, 4149–4169, https://doi.org/10.5194/amt-12-4149-2019, https://doi.org/10.5194/amt-12-4149-2019, 2019
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We present several changes to the setup of long-path differential optical absorption spectroscopy (LP-DOAS) instruments, including the application of a laser-driven light source, a modified coupling of the measurement signal between components, improved stray-light suppression, and better signal homogenization measures. These changes reduce detection limits of typical trace-gas species by a factor of 3–4 compared to previous setups and enable automated long-term observations in Antarctica.
Klaus Klingmüller, Jos Lelieveld, Vlassis A. Karydis, and Georgiy L. Stenchikov
Atmos. Chem. Phys., 19, 7397–7408, https://doi.org/10.5194/acp-19-7397-2019, https://doi.org/10.5194/acp-19-7397-2019, 2019
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Within the atmosphere, desert dust and anthropogenic pollution are mixed and interact, which affects the abundance and optical properties of the particulate matter. This results in an anthropogenic climate forcing associated with mineral dust notwithstanding the natural origin of most aeolian dust. With a global chemistry–climate model, we estimate this forcing to represent a considerable fraction of the total dust forcing.
Efstratios Bourtsoukidis, Lisa Ernle, John N. Crowley, Jos Lelieveld, Jean-Daniel Paris, Andrea Pozzer, David Walter, and Jonathan Williams
Atmos. Chem. Phys., 19, 7209–7232, https://doi.org/10.5194/acp-19-7209-2019, https://doi.org/10.5194/acp-19-7209-2019, 2019
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We report on results that demonstrate the utility of non-methane hydrocarbons as source/sink identification tracers while providing their mixing ratios around the Arabian Peninsula. By introducing novel data-analysis approaches, we establish a new method for separating associated and non-associated (with liquids) gases. We formulate a relationship between hydrocarbon oxidative pairs that can be used to evaluate the relative abundance of the hydroxyl and chlorine radicals in the troposphere.
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.
Meryem Tanarhte, Sara Bacer, Susannah M. Burrows, J. Alex Huffman, Kyle M. Pierce, Andrea Pozzer, Roland Sarda-Estève, Nicole J. Savage, and Jos Lelieveld
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2019-251, https://doi.org/10.5194/acp-2019-251, 2019
Publication in ACP not foreseen
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Bioaerosols have been an important topic in atmospheric science in the last two decades. This paper compares different emission parametrizations used in fungal spores modeling and compare their results to two sets of new observational datasets. It emphasises their uncertainties in order to improve their modeling in the future. This comparison is addressed primarily to the scientific community (publishing in ACP) interested in this type of modeling and the related experimental work in this field.
Rolf Sander, Andreas Baumgaertner, David Cabrera-Perez, Franziska Frank, Sergey Gromov, Jens-Uwe Grooß, Hartwig Harder, Vincent Huijnen, Patrick Jöckel, Vlassis A. Karydis, Kyle E. Niemeyer, Andrea Pozzer, Hella Riede, Martin G. Schultz, Domenico Taraborrelli, and Sebastian Tauer
Geosci. Model Dev., 12, 1365–1385, https://doi.org/10.5194/gmd-12-1365-2019, https://doi.org/10.5194/gmd-12-1365-2019, 2019
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We present the atmospheric chemistry box model CAABA/MECCA which
now includes a number of new features: skeletal mechanism
reduction, the MOM chemical mechanism for volatile organic
compounds, an option to include reactions from the Master
Chemical Mechanism (MCM) and other chemical mechanisms, updated
isotope tagging, improved and new photolysis modules, and the new
feature of coexisting multiple chemistry mechanisms.
CAABA/MECCA is a community model published under the GPL.
Philipp G. Eger, Frank Helleis, Gerhard Schuster, Gavin J. Phillips, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 12, 1935–1954, https://doi.org/10.5194/amt-12-1935-2019, https://doi.org/10.5194/amt-12-1935-2019, 2019
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We present a chemical ionization quadrupole mass spectrometer (CI-QMS) with a novel discharge ion source. In addition to the expected detection of PAN, peracetic acid and ClNO2, the instrument is also sensitive to SO2, HCl and acetic acid through ion chemistry unique for our ion source. We present ionization schemes along with illustrative datasets from field campaigns underlining the potential of the CI-QMS as an alternative to polonium, especially for application in the marine boundary layer.
Umar Javed, Dagmar Kubistin, Monica Martinez, Jan Pollmann, Markus Rudolf, Uwe Parchatka, Andreas Reiffs, Jim Thieser, Gerhard Schuster, Martin Horbanski, Denis Pöhler, John N. Crowley, Horst Fischer, Jos Lelieveld, and Hartwig Harder
Atmos. Meas. Tech., 12, 1461–1481, https://doi.org/10.5194/amt-12-1461-2019, https://doi.org/10.5194/amt-12-1461-2019, 2019
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Nitrogen dioxide (NO2) affects the concentration of key species like ozone, hydroxyl radical, and nitrate radical in the atmosphere. In situ, direct, and interference-free NO2 measurements are important for validating our understanding of NOx chemistry related to ozone formation and the radical loss process. This article describes the important features and performance of a newly developed NO2 instrument during a field intercomparison.
Guo Li, Yafang Cheng, Uwe Kuhn, Rongjuan Xu, Yudong Yang, Hannah Meusel, Zhibin Wang, Nan Ma, Yusheng Wu, Meng Li, Jonathan Williams, Thorsten Hoffmann, Markus Ammann, Ulrich Pöschl, Min Shao, and Hang Su
Atmos. Chem. Phys., 19, 2209–2232, https://doi.org/10.5194/acp-19-2209-2019, https://doi.org/10.5194/acp-19-2209-2019, 2019
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VOCs play a key role in atmospheric chemistry. Emission and deposition on soil have been suggested as important sources and sinks of atmospheric trace gases. The exchange characteristics and heterogeneous chemistry of VOCs on soil, however, are not well understood. We used a newly designed differential coated-wall flow tube system to investigate the long-term variability of bidirectional air–soil exchange of 13 VOCs at ambient air conditions of an urban background site in Beijing.
Laura Tomsche, Andrea Pozzer, Narendra Ojha, Uwe Parchatka, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 19, 1915–1939, https://doi.org/10.5194/acp-19-1915-2019, https://doi.org/10.5194/acp-19-1915-2019, 2019
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The Asian monsoon anticyclone (AMA) is an annual phenomenon in the northern hemispheric upper troposphere (UT) and lower stratosphere. We performed in situ measurements of carbon monoxide (CO) and methane (CH4) in the monsoon outflow region and in background air in the UT (Mediterranean, Arabian Peninsula, Arabian Sea) using airborne optical absorption spectroscopy during the Oxidation Mechanism Observations mission (summer 2015). The trace gases increased within the AMA, particularly CH4.
Yingying Yan, David Cabrera-Perez, Jintai Lin, Andrea Pozzer, Lu Hu, Dylan B. Millet, William C. Porter, and Jos Lelieveld
Geosci. Model Dev., 12, 111–130, https://doi.org/10.5194/gmd-12-111-2019, https://doi.org/10.5194/gmd-12-111-2019, 2019
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The GEOS-Chem model has been updated with the SAPRC-11 aromatics chemical mechanism to evaluate global and regional effects of aromatics on tropospheric oxidation capacity. Our results reveal relatively slight changes in ozone, hydroxyl radical, and nitrogen oxides on a global mean basis (1–4 %), although remarkable regional differences (5–20 %) exist near the source regions. Improved representation of aromatics is important to simulate the tropospheric oxidation.
Sebastian Ehrhart, Eimear M. Dunne, Hanna E. Manninen, Tuomo Nieminen, Jos Lelieveld, and Andrea Pozzer
Geosci. Model Dev., 11, 4987–5001, https://doi.org/10.5194/gmd-11-4987-2018, https://doi.org/10.5194/gmd-11-4987-2018, 2018
Christine D. Groot Zwaaftink, Stephan Henne, Rona L. Thompson, Edward J. Dlugokencky, Toshinobu Machida, Jean-Daniel Paris, Motoki Sasakawa, Arjo Segers, Colm Sweeney, and Andreas Stohl
Geosci. Model Dev., 11, 4469–4487, https://doi.org/10.5194/gmd-11-4469-2018, https://doi.org/10.5194/gmd-11-4469-2018, 2018
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A Lagrangian particle dispersion model is used to simulate global fields of methane, constrained by observations through nudging. We show that this rather simple and computationally inexpensive method can give results similar to or as good as a computationally expensive Eulerian chemistry transport model with a data assimilation scheme. The three-dimensional methane fields are of interest to applications such as inverse modelling and satellite retrievals.
Igor B. Konovalov, Daria A. Lvova, Matthias Beekmann, Hiren Jethva, Eugene F. Mikhailov, Jean-Daniel Paris, Boris D. Belan, Valerii S. Kozlov, Philippe Ciais, and Meinrat O. Andreae
Atmos. Chem. Phys., 18, 14889–14924, https://doi.org/10.5194/acp-18-14889-2018, https://doi.org/10.5194/acp-18-14889-2018, 2018
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A good knowledge of black carbon (BC) emissions from open biomass burning (BB) is an important prerequisite for reliable climate predictions, especially in the Arctic. This paper introduces a method to constrain a regional budget of BB BC emissions using satellite measurements of the absorption and extinction optical depths and evaluates its potential application in a large Siberian region.
Sara Bacer, Sylvia C. Sullivan, Vlassis A. Karydis, Donifan Barahona, Martina Krämer, Athanasios Nenes, Holger Tost, Alexandra P. Tsimpidi, Jos Lelieveld, and Andrea Pozzer
Geosci. Model Dev., 11, 4021–4041, https://doi.org/10.5194/gmd-11-4021-2018, https://doi.org/10.5194/gmd-11-4021-2018, 2018
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The complexity of ice nucleation mechanisms and aerosol--ice interactions makes their representation still challenging in atmospheric models. We have implemented a comprehensive ice crystal formation parameterization in the global chemistry-climate model EMAC to improve the representation of ice crystal number concentrations. The newly implemented parameterization takes into account processes which were previously neglected by the standard version of the model.
Terry J. Dillon and John N. Crowley
Atmos. Chem. Phys., 18, 14005–14015, https://doi.org/10.5194/acp-18-14005-2018, https://doi.org/10.5194/acp-18-14005-2018, 2018
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The reactions between electronically excited NO2* and NO3* with water vapour were studied using laser excitation of NO2 (532–647 nm) or NO3 (623–662 nm). No evidence for OH production was observed in either reaction. The reaction of NO2* with water is not a significant source of OH in the atmosphere.
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.
Jonathan M. Liebmann, Jennifer B. A. Muller, Dagmar Kubistin, Anja Claude, Robert Holla, Christian Plass-Dülmer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 18, 12045–12059, https://doi.org/10.5194/acp-18-12045-2018, https://doi.org/10.5194/acp-18-12045-2018, 2018
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We present direct measurements of the summertime total reactivity (inverse lifetime) of NO3 towards organic trace gases at a rural mountain site. High daytime and low night-time values were found. The reactivity was dominated by reaction with monoterpenes and sufficiently high to compete with photolysis and reaction with NO during daytime. NO3 radical measurements from one night are presented. For the first time, direct measurements of OH and NO3 reactivity are compared.
Alexandra P. Tsimpidi, Vlassis A. Karydis, Andrea Pozzer, Spyros N. Pandis, and Jos Lelieveld
Geosci. Model Dev., 11, 3369–3389, https://doi.org/10.5194/gmd-11-3369-2018, https://doi.org/10.5194/gmd-11-3369-2018, 2018
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A new module, ORACLE 2-D, that calculates the concentrations of surrogate organic species in two-dimensional space defined by volatility and oxygen-to-carbon ratio has been developed and evaluated. ORACLE 2-D uses a simple photochemical aging scheme that efficiently simulates the net effects of fragmentation and functionalization. ORACLE 2-D can be used to compute the ability of organic particles to act as cloud condensation nuclei and serves as a tool to quantify their climatic impact.
Zacharias Marinou Nikolaou, Jyh-Yuan Chen, Yiannis Proestos, Jos Lelieveld, and Rolf Sander
Geosci. Model Dev., 11, 3391–3407, https://doi.org/10.5194/gmd-11-3391-2018, https://doi.org/10.5194/gmd-11-3391-2018, 2018
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Chemistry is an important component of the atmosphere that describes many important physical processes. However, atmospheric chemical mechanisms include hundreds of species and reactions, posing a significant computational load. In this work, we use a powerful reduction method in order to develop a computationally faster chemical mechanism from a detailed mechanism. This enables accelerated simulations, which can be used to examine a wider range of processes in increased detail.
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.
Aristeidis K. Georgoulias, Athanasios Tsikerdekis, Vassilis Amiridis, Eleni Marinou, Angela Benedetti, Prodromos Zanis, Georgia Alexandri, Lucia Mona, Konstantinos A. Kourtidis, and Jos Lelieveld
Atmos. Chem. Phys., 18, 8601–8620, https://doi.org/10.5194/acp-18-8601-2018, https://doi.org/10.5194/acp-18-8601-2018, 2018
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In this work, the MACC reanalysis dust product is evaluated over Europe, Northern Africa and the Middle East using the EARLINET-optimized CALIOP/CALIPSO pure dust satellite-based product LIVAS (2007–2012). As dust plays a determinant role in processes related to weather and climate, human healt, and the economy, it is obvious that adequately simulating the amount of dust and its optical properties is essential. Our results could be used as a reference in future climate model evaluations.
Meryem Tanarhte, Sara Bacer, Susannah M. Burrows, J. Alex Huffman, Kyle M. Pierce, Andrea Pozzer, Roland Sarda-Estève, Nicole J. Savage, and Jos Lelieveld
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-361, https://doi.org/10.5194/acp-2018-361, 2018
Revised manuscript not accepted
Yingying Yan, Andrea Pozzer, Narendra Ojha, Jintai Lin, and Jos Lelieveld
Atmos. Chem. Phys., 18, 5589–5605, https://doi.org/10.5194/acp-18-5589-2018, https://doi.org/10.5194/acp-18-5589-2018, 2018
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Surface-based measurements from the EMEP network and EMAC model simulations are used to estimate the European surface ozone changes over 1995–2014. It shows a significantly decreasing trend in the 95th percentile ozone concentrations, while increasing in the 5th percentile ozone. Sensitivity simulations and statistical analysis show that a decrease in European anthropogenic emissions had contrasting effects on surface ozone trends between the 95th and 5th percentile levels.
Klaus Klingmüller, Swen Metzger, Mohamed Abdelkader, Vlassis A. Karydis, Georgiy L. Stenchikov, Andrea Pozzer, and Jos Lelieveld
Geosci. Model Dev., 11, 989–1008, https://doi.org/10.5194/gmd-11-989-2018, https://doi.org/10.5194/gmd-11-989-2018, 2018
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More than 1 billion tons of mineral dust particles are raised into the atmosphere every year, which has a significant impact on climate, society and ecosystems. The location, time and amount of dust emissions depend on surface and wind conditions. In the atmospheric chemistry–climate model EMAC, we have updated the relevant surface data and equations. Our validation shows that the updates substantially improve the agreement of model results and observations.
Jonathan Liebmann, Einar Karu, Nicolas Sobanski, Jan Schuladen, Mikael Ehn, Simon Schallhart, Lauriane Quéléver, Heidi Hellen, Hannele Hakola, Thorsten Hoffmann, Jonathan Williams, Horst Fischer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 18, 3799–3815, https://doi.org/10.5194/acp-18-3799-2018, https://doi.org/10.5194/acp-18-3799-2018, 2018
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Using a newly developed experimental setup, we have made the first direct measurements (during autumn 2016) of NO3 reactivity in the Finnish boreal forest. The NO3 reactivity was generally very high (maximum value of 0.94/s) so that daytime reaction with organics was a substantial fraction of the NO3 loss. Observations of biogenic hydrocarbons (BVOCs) suggested a dominant role for monoterpenes in determining the NO3 reactivity, which displayed a strong vertical gradient between 8.5 and 25 m.
Ana María Yáñez-Serrano, Anke Christine Nölscher, Efstratios Bourtsoukidis, Eliane Gomes Alves, Laurens Ganzeveld, Boris Bonn, Stefan Wolff, Marta Sa, Marcia Yamasoe, Jonathan Williams, Meinrat O. Andreae, and Jürgen Kesselmeier
Atmos. Chem. Phys., 18, 3403–3418, https://doi.org/10.5194/acp-18-3403-2018, https://doi.org/10.5194/acp-18-3403-2018, 2018
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This study shows the measurements of concentration of different monoterpene species in terms of height, time of day and season. Speciation seems similar during the dry seasons but changes with season. Furthermore, reactivity with the different oxidants demonstrated that a higher abundance of a monoterpene species does not automatically imply higher reactivity and that the most abundant monoterpene may not be the most atmospheric chemically relevant compound.
Katrin Dulitz, Damien Amedro, Terry J. Dillon, Andrea Pozzer, and John N. Crowley
Atmos. Chem. Phys., 18, 2381–2394, https://doi.org/10.5194/acp-18-2381-2018, https://doi.org/10.5194/acp-18-2381-2018, 2018
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The reaction between the OH radical and HNO3 represents an important route for the release of NOx (NO and NO2) from HNO3, the most important NOx reservoir in many parts of the atmosphere. In our laboratory study, we have generated an extensive, high-quality set of rate coefficients for this reaction at different temperatures and pressures and used these to derive a new parameterisation of the rate coefficient for atmospheric modelling.
George K. Georgiou, Theodoros Christoudias, Yiannis Proestos, Jonilda Kushta, Panos Hadjinicolaou, and Jos Lelieveld
Atmos. Chem. Phys., 18, 1555–1571, https://doi.org/10.5194/acp-18-1555-2018, https://doi.org/10.5194/acp-18-1555-2018, 2018
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We investigate the impact of the choice of gas-phase and aerosol mechanisms, on the simulated summertime concentrations of several pollutants over the eastern Mediterranean, using the WRF-Chem model. The selection of mechanisms significantly affects ozone and fine particulate matter concentrations, and to a lesser extent other gaseous pollutants (NOx, CO). Meteorological components are also affected by the choice of mechanisms due to the interaction of aerosols with radiation.
Hannah Meusel, Alexandra Tamm, Uwe Kuhn, Dianming Wu, Anna Lena Leifke, Sabine Fiedler, Nina Ruckteschler, Petya Yordanova, Naama Lang-Yona, Mira Pöhlker, Jos Lelieveld, Thorsten Hoffmann, Ulrich Pöschl, Hang Su, Bettina Weber, and Yafang Cheng
Atmos. Chem. Phys., 18, 799–813, https://doi.org/10.5194/acp-18-799-2018, https://doi.org/10.5194/acp-18-799-2018, 2018
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The photolysis of nitrous acid (HONO) forms the OH radical. However, not all sources are known. Recent studies showed that HONO can be emitted from soil but they did not evaluate the importance to the HONO budget. In this work HONO emissions from 43 soil and biological soil crust samples from Cyprus were measured in a dynamic chamber and extrapolated to the real atmosphere. A large fraction of the local missing source (published earlier; Meusel et al., 2016) could be assigned to soil emissions.
Efstratios Bourtsoukidis, Frank Helleis, Laura Tomsche, Horst Fischer, Rolf Hofmann, Jos Lelieveld, and Jonathan Williams
Atmos. Meas. Tech., 10, 5089–5105, https://doi.org/10.5194/amt-10-5089-2017, https://doi.org/10.5194/amt-10-5089-2017, 2017
Terry J. Dillon, Katrin Dulitz, Christoph B. M. Groß, and John N. Crowley
Atmos. Chem. Phys., 17, 15137–15150, https://doi.org/10.5194/acp-17-15137-2017, https://doi.org/10.5194/acp-17-15137-2017, 2017
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A great quantity and variety of organic compounds is released to the atmosphere annually. These compounds greatly impact air chemistry, quality and climate. Laser-based experiments were used to study the atmospheric breakdown of three organics: isoprene, alpha-pinene, and delta-3-carene. Results provided important missing information for low-temperature atmospheric conditions, resolved discrepancies from previous work, and allowed estimation of lifetimes of a few hours for each compound.
Gabriella M. Weiss, Eva Y. Pfannerstill, Stefan Schouten, Jaap S. Sinninghe Damsté, and Marcel T. J. van der Meer
Biogeosciences, 14, 5693–5704, https://doi.org/10.5194/bg-14-5693-2017, https://doi.org/10.5194/bg-14-5693-2017, 2017
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Algal-derived compounds allow us to make assumptions about environmental conditions in the past. In order to better understand how organisms record environmental conditions, we grew microscopic marine algae at different light intensities, salinities, and alkalinities in a temperature-controlled environment. We determined how these environmental parameters affected specific algal-derived compounds, especially their relative deuterium content, which seems to be mainly affected by salinity.
Amit Sharma, Narendra Ojha, Andrea Pozzer, Kathleen A. Mar, Gufran Beig, Jos Lelieveld, and Sachin S. Gunthe
Atmos. Chem. Phys., 17, 14393–14413, https://doi.org/10.5194/acp-17-14393-2017, https://doi.org/10.5194/acp-17-14393-2017, 2017
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We evaluate the numerical simulations of surface ozone during pre-monsoon season against a network of stations including clean, rural and polluted urban environments in the south Asian region. Significant effects of the employed emission inventory and chemical mechanism on the simulated ozone are found during the noon hours of intense photochemistry. The presented evaluation on the diurnal timescale would have implications for assessing ozone buildup and impacts on human health and crop yields.
Andrea Pozzer, Alexandra P. Tsimpidi, Vlassis A. Karydis, Alexander de Meij, and Jos Lelieveld
Atmos. Chem. Phys., 17, 12813–12826, https://doi.org/10.5194/acp-17-12813-2017, https://doi.org/10.5194/acp-17-12813-2017, 2017
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This study shows that agricultural emissions are important for air quality and their reduction can effectively reduce the concentration of fine particles and their associated premature mortality. Therefore, emission control policies, especially in North America and Europe, should also involve strong ammonia emission decreases to optimally reduce fine-particle concentration.
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).
David Cabrera-Perez, Domenico Taraborrelli, Jos Lelieveld, Thorsten Hoffmann, and Andrea Pozzer
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2017-928, https://doi.org/10.5194/acp-2017-928, 2017
Revised manuscript not accepted
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Aromatic compounds are present in rural and urban atmospheres. The aim of this work is to disentangle the impacts of these compounds in different important atmospheric chemical species with the help of a numerical model. Aromatics have low impact OH, NOx and Ozone concentrations in the global scale (below 4 %). The impact however is larger in the regional scale (up to 10 %). The largest impact is in glyoxal and NO3 concentrations, with changes up to 10 % globally and 40 % regionally.
Heiko Bozem, Andrea Pozzer, Hartwig Harder, Monica Martinez, Jonathan Williams, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 17, 11835–11848, https://doi.org/10.5194/acp-17-11835-2017, https://doi.org/10.5194/acp-17-11835-2017, 2017
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We present a case study of deep convection over Germany in July 2007 within the framework of the HOOVER II project. Airborne in situ measurements within the in- and outflow regions of an isolated thunderstorm provide a unique data set to study the influence of deep convection on the transport efficiency of soluble and insoluble trace gases. Despite their high solubility HCHO and H2O2 show enhanced concentrations in the outflow presumably due to degassing from cloud droplets during freezing.
Hannah Meusel, Yasin Elshorbany, Uwe Kuhn, Thorsten Bartels-Rausch, Kathrin Reinmuth-Selzle, Christopher J. Kampf, Guo Li, Xiaoxiang Wang, Jos Lelieveld, Ulrich Pöschl, Thorsten Hoffmann, Hang Su, Markus Ammann, and Yafang Cheng
Atmos. Chem. Phys., 17, 11819–11833, https://doi.org/10.5194/acp-17-11819-2017, https://doi.org/10.5194/acp-17-11819-2017, 2017
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In this study we investigated protein nitration and decomposition by light in the presence of NO2 via flow tube measurements. Nitrated proteins have an enhanced allergenic potential but so far nitration was only studied in dark conditions. Under irradiated conditions we found that proteins predominantly decompose while forming nitrous acid (HONO) an important precursor of the OH radical. Unlike other studies on heterogeneous NO2 conversion we found a stable HONO formation over a long period.
Imke Hüser, Hartwig Harder, Angelika Heil, and Johannes W. Kaiser
Atmos. Chem. Phys., 17, 10955–10967, https://doi.org/10.5194/acp-17-10955-2017, https://doi.org/10.5194/acp-17-10955-2017, 2017
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The impact of pollution sources on downwind sites can be quantified by Lagrangian dispersion models. We identified the representation of the mixing layer dynamics as a crucial factor for the vertical mixing of surface pollutants. Our application examples show that inaccuracies may introduce errors in the impact assessment on downwind sites. For vegetation fires, mixing by pyrogenic convection is under-represented. We find an overestimation of downwind smoke concentration of more than 60 %.
Heiko Bozem, Tim M. Butler, Mark G. Lawrence, Hartwig Harder, Monica Martinez, Dagmar Kubistin, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 17, 10565–10582, https://doi.org/10.5194/acp-17-10565-2017, https://doi.org/10.5194/acp-17-10565-2017, 2017
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We present airborne measurements and model simulations in the tropics and mid-latitudes during GABRIEL and HOOVER, respectively. Based only on in situ data net ozone formation/destruction tendencies (NOPR) are calculated and compared to a 3-D chemistry transport model. The NOPR is positive in the continental boundary layer and the upper troposphere above 6 km. In the marine boundary layer and the middle troposphere ozone destruction prevails. Fresh convection shows strong net ozone formation.
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.
Stephan Keßel, David Cabrera-Perez, Abraham Horowitz, Patrick R. Veres, Rolf Sander, Domenico Taraborrelli, Maria Tucceri, John N. Crowley, Andrea Pozzer, Christof Stönner, Luc Vereecken, Jos Lelieveld, and Jonathan Williams
Atmos. Chem. Phys., 17, 8789–8804, https://doi.org/10.5194/acp-17-8789-2017, https://doi.org/10.5194/acp-17-8789-2017, 2017
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In this study we identify an often overlooked stable oxide of carbon, namely carbon suboxide (C3O2), in ambient air. We have made C3O2 and in the laboratory determined its absorption cross section data and the rate of reaction with two important atmospheric oxidants, OH and O3. By incorporating known sources and sinks in a global model we have generated a first global picture of the distribution of this species in the atmosphere.
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.
Alexandra P. Tsimpidi, Vlassis A. Karydis, Spyros N. Pandis, and Jos Lelieveld
Atmos. Chem. Phys., 17, 7345–7364, https://doi.org/10.5194/acp-17-7345-2017, https://doi.org/10.5194/acp-17-7345-2017, 2017
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We analyzed the sensitivity of model-predicted global-scale OA to parameters and assumptions that control primary emissions, photochemical aging, and the scavenging efficiency of LVOCs, SVOCs, and IVOCs. The simulated OA concentrations were evaluated against a global dataset of AMS measurements. According to our analysis, a combination of increased IVOCs and decreased hygroscopicity of the freshly emitted IVOCs can help reduce discrepancies between simulated SOA and observed OOA concentrations.
Yudong Yang, Min Shao, Stephan Keßel, Yue Li, Keding Lu, Sihua Lu, Jonathan Williams, Yuanhang Zhang, Liming Zeng, Anke C. Nölscher, Yusheng Wu, Xuemei Wang, and Junyu Zheng
Atmos. Chem. Phys., 17, 7127–7142, https://doi.org/10.5194/acp-17-7127-2017, https://doi.org/10.5194/acp-17-7127-2017, 2017
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Total OH reactivity is an important parameter to evaluate understanding of atmospheric chemistry, especially the VOC contribution to air pollution. Measured by comparative reactivity methods, total OH reactivity in Beijing and Heshan revealed significant differences between measured and calculated results, such as missing reactivity, which were related to unmeasured primary or secondary species. This missing reactivity would introduce a 21–30 % underestimation for ozone production efficiency.
Narendra Ojha, Andrea Pozzer, Dimitris Akritidis, and Jos Lelieveld
Atmos. Chem. Phys., 17, 6743–6757, https://doi.org/10.5194/acp-17-6743-2017, https://doi.org/10.5194/acp-17-6743-2017, 2017
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We investigate the processes, frequency of occurrence and seasonality, and effects of strongly enhanced ozone layers in the middle–upper troposphere (SOPs) over the Himalayas using a global model (EMAC). Rapid transport of stratospheric air masses is found as a key underlying process. Model predicts more frequent SOP events during the pre-monsoon. SOPs are found to significantly enhance the tropospheric ozone column over the Himalayas.
Vlassis A. Karydis, Alexandra P. Tsimpidi, Sara Bacer, Andrea Pozzer, Athanasios Nenes, and Jos Lelieveld
Atmos. Chem. Phys., 17, 5601–5621, https://doi.org/10.5194/acp-17-5601-2017, https://doi.org/10.5194/acp-17-5601-2017, 2017
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The importance of mineral dust for cloud droplet formation is studied by considering the adsorption activation of insoluble dust particles and the thermodynamic interactions between mineral cations and inorganic anions. This study demonstrates that a comprehensive treatment of the CCN activity of mineral dust and its chemical and thermodynamic interactions with inorganic species by chemistry climate models is important to realistically account for aerosol–chemistry–cloud–climate interaction.
Jonathan M. Liebmann, Gerhard Schuster, Jan B. Schuladen, Nicolas Sobanski, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 10, 1241–1258, https://doi.org/10.5194/amt-10-1241-2017, https://doi.org/10.5194/amt-10-1241-2017, 2017
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We describe the first instrument for measurement of the rate constant for reactive loss (i.e. the total reactivity) of NO3 in ambient air. This is essentially a measureement of the lifetime of NO3 and will help assess the role of NO3 and N2O5 in conversion of reactive nitrogen oxides to reservoir species in the troposphere.
Nicolas Sobanski, Jim Thieser, Jan Schuladen, Carina Sauvage, Wei Song, Jonathan Williams, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 17, 4115–4130, https://doi.org/10.5194/acp-17-4115-2017, https://doi.org/10.5194/acp-17-4115-2017, 2017
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We investigated the formation of gas-phase organic nitrates at a forested semi-urban site. This work constitutes the first detailed analysis of the sum of organic nitrate mixing ratios measured by thermal dissociation cavity ring-down spectroscopy in continental Europe. Day (OH-initiated) and night-time (NO3-initiated) production of alkyl nitrates proceed at similar rates.
Mohamed Abdelkader, Swen Metzger, Benedikt Steil, Klaus Klingmüller, Holger Tost, Andrea Pozzer, Georgiy Stenchikov, Leonard Barrie, and Jos Lelieveld
Atmos. Chem. Phys., 17, 3799–3821, https://doi.org/10.5194/acp-17-3799-2017, https://doi.org/10.5194/acp-17-3799-2017, 2017
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We present a modeling study on the impacts of the key processes (dust emission flux, convection and dust aging parameterizations) that control the transatlantic dust transport using an advanced version of the EMAC atmospheric chemistry general circulation model. We define the
direct effect of dust agingas an increase in the AOD as a result of hygroscopic growth. We define the
indirect effectas a reduction in the dust AOD due to the higher removal of the aged dust particles.
Saehee Lim, Xavier Faïn, Patrick Ginot, Vladimir Mikhalenko, Stanislav Kutuzov, Jean-Daniel Paris, Anna Kozachek, and Paolo Laj
Atmos. Chem. Phys., 17, 3489–3505, https://doi.org/10.5194/acp-17-3489-2017, https://doi.org/10.5194/acp-17-3489-2017, 2017
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A record of light-absorbing refractory black carbon (rBC), emitted by fossil fuel combustion and biomass burning, was reconstructed from the ice cores drilled at a high-altitude eastern European site in Mt. Elbrus. This record reports for the first time the high-resolution rBC mass concentrations in the European outflows over the past 189 years. Our study suggests that the past changes in BC emissions of eastern Europe need to be considered in assessing ongoing air quality regulations.
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.
Imran A. Girach, Narendra Ojha, Prabha R. Nair, Andrea Pozzer, Yogesh K. Tiwari, K. Ravi Kumar, and Jos Lelieveld
Atmos. Chem. Phys., 17, 257–275, https://doi.org/10.5194/acp-17-257-2017, https://doi.org/10.5194/acp-17-257-2017, 2017
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This study presents first ship-borne measurements of trace gases over the Bay of Bengal during summer monsoon. The observed variations in trace gases are shown to be due to dynamics/transport and en route photochemistry. Analysis of meteorological and chemical fields shows that significantly lower ozone during rainfall is associated with the downdrafts. A regional model reproduces the observed variations and revealed the rapid transport of ozone across the Bay of Bengal during an event.
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.
Dimitris Akritidis, Andrea Pozzer, Prodromos Zanis, Evangelos Tyrlis, Bojan Škerlak, Michael Sprenger, and Jos Lelieveld
Atmos. Chem. Phys., 16, 14025–14039, https://doi.org/10.5194/acp-16-14025-2016, https://doi.org/10.5194/acp-16-14025-2016, 2016
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We investigate the contribution of tropopause folds in the summertime tropospheric ozone pool over the eastern Mediterranean and the Middle East. For this purpose we use the EMAC atmospheric chemistry–climate model and a fold identification algorithm. A clear increase of ozone is found in the middle troposphere due to fold activity. The interannual variability of near-surface ozone over the eastern Mediterranean is related to that of both tropopause folds and ozone in the free troposphere.
Aristeidis K. Georgoulias, Georgia Alexandri, Konstantinos A. Kourtidis, Jos Lelieveld, Prodromos Zanis, Ulrich Pöschl, Robert Levy, Vassilis Amiridis, Eleni Marinou, and Athanasios Tsikerdekis
Atmos. Chem. Phys., 16, 13853–13884, https://doi.org/10.5194/acp-16-13853-2016, https://doi.org/10.5194/acp-16-13853-2016, 2016
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In this work, single pixel observations from MODIS Terra and Aqua are analyzed together with data from other satellite sensors, reanalysis projects and a chemistry–aerosol-transport model to study the spatiotemporal variability of different aerosol types. The results are in accordance with previous works and are a good reference for future studies in the area focusing on aerosols, clouds, radiation and the effects of particle pollution on human health.
Gavin J. Phillips, Jim Thieser, Mingjin Tang, Nicolas Sobanski, Gerhard Schuster, Johannes Fachinger, Frank Drewnick, Stephan Borrmann, Heinz Bingemer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 16, 13231–13249, https://doi.org/10.5194/acp-16-13231-2016, https://doi.org/10.5194/acp-16-13231-2016, 2016
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We use trace gas measurements (N2O5, ClNO2, NO3) and particle properties (surface area, nitrate content etc.) to derive uptake coefficients (the probability of removal from the gas-phase on a per-collision basis) for the interaction of N2O5 with ambient aerosol and also the efficiency of formation of ClNO2. The uptake coefficients show high variability but are reasonably well captured by parameterisations based on laboratory measurements.
Nicolas Sobanski, Jan Schuladen, Gerhard Schuster, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 9, 5103–5118, https://doi.org/10.5194/amt-9-5103-2016, https://doi.org/10.5194/amt-9-5103-2016, 2016
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We report the characteristics and performances of a cavity ring-down spectrometer (CRDS) designed for field measurements that uses light absorption at 662 and 405 nm to detect different reactive nitrogen species or group of species in the gas phase, either directly or after thermal decomposition. We report improvements compared to currently existing instruments, and describe the corrections applied to the raw data to account for chemical and optical interferences.
Jos Lelieveld, Sergey Gromov, Andrea Pozzer, and Domenico Taraborrelli
Atmos. Chem. Phys., 16, 12477–12493, https://doi.org/10.5194/acp-16-12477-2016, https://doi.org/10.5194/acp-16-12477-2016, 2016
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The self-cleaning capacity of the atmosphere is controlled by hydroxyl (OH) radicals in the troposphere. There are primary and secondary OH sources, the former through the photodissociation of ozone, the latter through OH recycling. We used a global model, showing that secondary sources are larger than assumed previously, which buffers OH. Complementary OH formation mechanisms in pristine and polluted environments, connected through transport of ozone, can maintain stable global OH levels.
A. M. Yáñez-Serrano, A. C. Nölscher, E. Bourtsoukidis, B. Derstroff, N. Zannoni, V. Gros, M. Lanza, J. Brito, S. M. Noe, E. House, C. N. Hewitt, B. Langford, E. Nemitz, T. Behrendt, J. Williams, P. Artaxo, M. O. Andreae, and J. Kesselmeier
Atmos. Chem. Phys., 16, 10965–10984, https://doi.org/10.5194/acp-16-10965-2016, https://doi.org/10.5194/acp-16-10965-2016, 2016
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This paper provides a general overview of methyl ethyl ketone (MEK) ambient observations in different ecosystems around the world in order to provide insights into the sources, sink and role of MEK in the atmosphere.
Jan Zörner, Marloes Penning de Vries, Steffen Beirle, Holger Sihler, Patrick R. Veres, Jonathan Williams, and Thomas Wagner
Atmos. Chem. Phys., 16, 9457–9487, https://doi.org/10.5194/acp-16-9457-2016, https://doi.org/10.5194/acp-16-9457-2016, 2016
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We present a top-down approach to infer and quantify rain-induced emission pulses of nitrogen oxides from soils using satellite-borne measurements of NO2. We found strong enhancements of NO2 induced by the first intense precipitation after prolonged droughts in many semi-arid regions of the world, in particular in the Sahel. Apart from the clear first-day peak, NO2 VCDs are moderately enhanced compared to background over the following 2 weeks suggesting potential further emissions.
Alexandra P. Tsimpidi, Vlassis A. Karydis, Spyros N. Pandis, and Jos Lelieveld
Atmos. Chem. Phys., 16, 8939–8962, https://doi.org/10.5194/acp-16-8939-2016, https://doi.org/10.5194/acp-16-8939-2016, 2016
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In this work we use a global chemistry climate model together with a comprehensive global AMS data set in order to provide valuable insights into the temporal and geographical variability of the contribution of the emitted particles and the chemically processed organic material from combustion sources to total OA. This study reveals the high importance of SOA from anthropogenic sources on global OA concentrations and identifies plausible sources of discrepancy between models and measurements.
Swen Metzger, Benedikt Steil, Mohamed Abdelkader, Klaus Klingmüller, Li Xu, Joyce E. Penner, Christos Fountoukis, Athanasios Nenes, and Jos Lelieveld
Atmos. Chem. Phys., 16, 7213–7237, https://doi.org/10.5194/acp-16-7213-2016, https://doi.org/10.5194/acp-16-7213-2016, 2016
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We introduce an unique single parameter framework to efficiently parameterize the aerosol water uptake for mixtures of semi-volatile and non-volatile compounds, being entirely based on the single solute specific coefficient introduced in Metzger et al. (2012).
Klaus Klingmüller, Andrea Pozzer, Swen Metzger, Georgiy L. Stenchikov, and Jos Lelieveld
Atmos. Chem. Phys., 16, 5063–5073, https://doi.org/10.5194/acp-16-5063-2016, https://doi.org/10.5194/acp-16-5063-2016, 2016
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During the last decade, the Middle East experienced the strongest increase in atmospheric aerosol concentrations worldwide. Based on satellite observations, the present study corroborates this trend and reveals correlations with soil moisture and precipitation in and surrounding the Fertile Crescent. This suggests that the increasing drought conditions in this region have enhanced dust emissions, a tendency which is expected to be intensified by climate change.
N. Sobanski, M. J. Tang, J. Thieser, G. Schuster, D. Pöhler, H. Fischer, W. Song, C. Sauvage, J. Williams, J. Fachinger, F. Berkes, P. Hoor, U. Platt, J. Lelieveld, and J. N. Crowley
Atmos. Chem. Phys., 16, 4867–4883, https://doi.org/10.5194/acp-16-4867-2016, https://doi.org/10.5194/acp-16-4867-2016, 2016
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The nitrate radical (NO3) is an important nocturnal oxidant. By measuring NO3, its precursors (nitrogen dioxide and ozone) and several trace gases with which it reacts, we examined the chemical and meteorological factors influencing the lifetime of NO3 at a semi-rural mountain site. Unexpectedly long lifetimes, approaching 1 h, were observed on several nights and were associated with a low-lying residual layer. We discuss the role of other reactions that convert NO2 to NO3.
Armin Rauthe-Schöch, Angela K. Baker, Tanja J. Schuck, Carl A. M. Brenninkmeijer, Andreas Zahn, Markus Hermann, Greta Stratmann, Helmut Ziereis, Peter F. J. van Velthoven, and Jos Lelieveld
Atmos. Chem. Phys., 16, 3609–3629, https://doi.org/10.5194/acp-16-3609-2016, https://doi.org/10.5194/acp-16-3609-2016, 2016
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The flying laboratory CARIBIC onboard a passenger aircraft measured trace gases and aerosol particles in the upper tropospheric Indian summer monsoon anticyclone in summer 2008. We used the measurements together with meteorological analyses to investigate the chemical signature of the northern and southern part of the monsoon, the source regions from where the air was entrained into the monsoon and which parts of the world received polluted air that had been chemically processed in the monsoon.
Narendra Ojha, Andrea Pozzer, Armin Rauthe-Schöch, Angela K. Baker, Jongmin Yoon, Carl A. M. Brenninkmeijer, and Jos Lelieveld
Atmos. Chem. Phys., 16, 3013–3032, https://doi.org/10.5194/acp-16-3013-2016, https://doi.org/10.5194/acp-16-3013-2016, 2016
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We compare simulations of ozone and carbon monoxide using a regional chemistry transport model (WRF-Chem) with aircraft observations from CARIBIC program over India during monsoon period. Sensitivity simulations are conducted to assess the influences of regional emissions and long-range transport.
J. Thieser, G. Schuster, J. Schuladen, G. J. Phillips, A. Reiffs, U. Parchatka, D. Pöhler, J. Lelieveld, and J. N. Crowley
Atmos. Meas. Tech., 9, 553–576, https://doi.org/10.5194/amt-9-553-2016, https://doi.org/10.5194/amt-9-553-2016, 2016
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We report on the use of thermal dissociation cavity ring-down spectroscopy to detect NO2, peroxy nitrates and alkyl nitrates. We present both laboratory studies that characterise the chemical formation and loss of NO2 in the heated inlets and also result from a first field deployment.
V. A. Karydis, A. P. Tsimpidi, A. Pozzer, M. Astitha, and J. Lelieveld
Atmos. Chem. Phys., 16, 1491–1509, https://doi.org/10.5194/acp-16-1491-2016, https://doi.org/10.5194/acp-16-1491-2016, 2016
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We provide an assessment of the chemical composition and global aerosol load of aerosol nitrate and determine the effect of mineral dust on its formation due to thermodynamical interactions. For this purpose we used an explicit geographical representation of the emitted soil particle size distribution and chemical composition. We conclude mineral dust aerosol chemistry is important for nitrate aerosol formation and significantly affects its global distribution, especially in the coarse mode.
M. O. Andreae, O. C. Acevedo, A. Araùjo, P. Artaxo, C. G. G. Barbosa, H. M. J. Barbosa, J. Brito, S. Carbone, X. Chi, B. B. L. Cintra, N. F. da Silva, N. L. Dias, C. Q. Dias-Júnior, F. Ditas, R. Ditz, A. F. L. Godoi, R. H. M. Godoi, M. Heimann, T. Hoffmann, J. Kesselmeier, T. Könemann, M. L. Krüger, J. V. Lavric, A. O. Manzi, A. P. Lopes, D. L. Martins, E. F. Mikhailov, D. Moran-Zuloaga, B. W. Nelson, A. C. Nölscher, D. Santos Nogueira, M. T. F. Piedade, C. Pöhlker, U. Pöschl, C. A. Quesada, L. V. Rizzo, C.-U. Ro, N. Ruckteschler, L. D. A. Sá, M. de Oliveira Sá, C. B. Sales, R. M. N. dos Santos, J. Saturno, J. Schöngart, M. Sörgel, C. M. de Souza, R. A. F. de Souza, H. Su, N. Targhetta, J. Tóta, I. Trebs, S. Trumbore, A. van Eijck, D. Walter, Z. Wang, B. Weber, J. Williams, J. Winderlich, F. Wittmann, S. Wolff, and A. M. Yáñez-Serrano
Atmos. Chem. Phys., 15, 10723–10776, https://doi.org/10.5194/acp-15-10723-2015, https://doi.org/10.5194/acp-15-10723-2015, 2015
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This paper describes the Amazon Tall Tower Observatory (ATTO), a new atmosphere-biosphere observatory located in the remote Amazon Basin. It presents results from ecosystem ecology, meteorology, trace gas, and aerosol measurements collected at the ATTO site during the first 3 years of operation.
M. Abdelkader, S. Metzger, R. E. Mamouri, M. Astitha, L. Barrie, Z. Levin, and J. Lelieveld
Atmos. Chem. Phys., 15, 9173–9189, https://doi.org/10.5194/acp-15-9173-2015, https://doi.org/10.5194/acp-15-9173-2015, 2015
H. G. Ouwersloot, A. Pozzer, B. Steil, H. Tost, and J. Lelieveld
Geosci. Model Dev., 8, 2435–2445, https://doi.org/10.5194/gmd-8-2435-2015, https://doi.org/10.5194/gmd-8-2435-2015, 2015
H. Fischer, A. Pozzer, T. Schmitt, P. Jöckel, T. Klippel, D. Taraborrelli, and J. Lelieveld
Atmos. Chem. Phys., 15, 6971–6980, https://doi.org/10.5194/acp-15-6971-2015, https://doi.org/10.5194/acp-15-6971-2015, 2015
K. Violaki, J. Sciare, J. Williams, A. R. Baker, M. Martino, and N. Mihalopoulos
Biogeosciences, 12, 3131–3140, https://doi.org/10.5194/bg-12-3131-2015, https://doi.org/10.5194/bg-12-3131-2015, 2015
S. Zheng, A. Pozzer, C. X. Cao, and J. Lelieveld
Atmos. Chem. Phys., 15, 5715–5725, https://doi.org/10.5194/acp-15-5715-2015, https://doi.org/10.5194/acp-15-5715-2015, 2015
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The present study uses aerosol optical depth as proxy to estimate 12 years of PM2.5 data for the Beijing central area and calculate the yearly premature mortality by different diseases attributable to PM2.5. The estimated average total mortality due to PM2.5 is about 5100 individuals/year for the period 2001--2012 in the Beijing central area, and the per capita mortality for all ages due to PM2.5 is around 15 per 10,000 person-years for the period 2010--2012.
D. Mogensen, R. Gierens, J. N. Crowley, P. Keronen, S. Smolander, A. Sogachev, A. C. Nölscher, L. Zhou, M. Kulmala, M. J. Tang, J. Williams, and M. Boy
Atmos. Chem. Phys., 15, 3909–3932, https://doi.org/10.5194/acp-15-3909-2015, https://doi.org/10.5194/acp-15-3909-2015, 2015
A. M. Yáñez-Serrano, A. C. Nölscher, J. Williams, S. Wolff, E. Alves, G. A. Martins, E. Bourtsoukidis, J. Brito, K. Jardine, P. Artaxo, and J. Kesselmeier
Atmos. Chem. Phys., 15, 3359–3378, https://doi.org/10.5194/acp-15-3359-2015, https://doi.org/10.5194/acp-15-3359-2015, 2015
E. Mesarchaki, C. Kräuter, K. E. Krall, M. Bopp, F. Helleis, J. Williams, and B. Jähne
Ocean Sci., 11, 121–138, https://doi.org/10.5194/os-11-121-2015, https://doi.org/10.5194/os-11-121-2015, 2015
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Our article presents successful gas exchange measurements obtained in a large-scale wind-wave tank. The adopted box model methodology, experimental produce and instrumentation are described in detail. For the first time, parallel measurements of total transfer velocities for 14 individual gases within a wide range of solubility have been achieved. Various wind speed conditions and the effect of surfactant layers have been investigated providing exciting results.
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. E. Stockwell, P. R. Veres, J. Williams, and R. J. Yokelson
Atmos. Chem. Phys., 15, 845–865, https://doi.org/10.5194/acp-15-845-2015, https://doi.org/10.5194/acp-15-845-2015, 2015
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We used a high-resolution proton-transfer-reaction time-of-flight mass spectrometer to measure emissions from peat, crop residue, cooking fires, etc. We assigned > 80% of the mass of gas-phase organic compounds and much of it was secondary organic aerosol precursors. The open cooking emissions were much larger than from advanced cookstoves. Little-studied N-containing organic compounds accounted for 0.1-8.7% of the fuel N and may influence new particle formation.
A. P. Tsimpidi, V. A. Karydis, A. Pozzer, S. N. Pandis, and J. Lelieveld
Geosci. Model Dev., 7, 3153–3172, https://doi.org/10.5194/gmd-7-3153-2014, https://doi.org/10.5194/gmd-7-3153-2014, 2014
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A computationally efficient module for the description of OA composition and evolution in the atmosphere has been developed. This module subdivides OA into several compounds based on their source of origin and volatility, allowing the quantification of POA vs. SOA as well as biogenic vs. anthropogenic contributions to OA concentrations. Such fundamental information can shed light on long-term changes in OA abundance, and hence project the effects of OA on future air quality and climate.
K. Klingmüller, B. Steil, C. Brühl, H. Tost, and J. Lelieveld
Geosci. Model Dev., 7, 2503–2516, https://doi.org/10.5194/gmd-7-2503-2014, https://doi.org/10.5194/gmd-7-2503-2014, 2014
B. Bonn, E. Bourtsoukidis, T. S. Sun, H. Bingemer, L. Rondo, U. Javed, J. Li, R. Axinte, X. Li, T. Brauers, H. Sonderfeld, R. Koppmann, A. Sogachev, S. Jacobi, and D. V. Spracklen
Atmos. Chem. Phys., 14, 10823–10843, https://doi.org/10.5194/acp-14-10823-2014, https://doi.org/10.5194/acp-14-10823-2014, 2014
T. Behrendt, P. R. Veres, F. Ashuri, G. Song, M. Flanz, B. Mamtimin, M. Bruse, J. Williams, and F. X. Meixner
Biogeosciences, 11, 5463–5492, https://doi.org/10.5194/bg-11-5463-2014, https://doi.org/10.5194/bg-11-5463-2014, 2014
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
H. Bozem, H. Fischer, C. Gurk, C. L. Schiller, U. Parchatka, R. Koenigstedt, A. Stickler, M. Martinez, H. Harder, D. Kubistin, J. Williams, G. Eerdekens, and J. Lelieveld
Atmos. Chem. Phys., 14, 8917–8931, https://doi.org/10.5194/acp-14-8917-2014, https://doi.org/10.5194/acp-14-8917-2014, 2014
D. Y. Chang, H. Tost, B. Steil, and J. Lelieveld
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-14-21975-2014, https://doi.org/10.5194/acpd-14-21975-2014, 2014
Preprint withdrawn
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
P. R. Veres, T. Behrendt, A. Klapthor, F. X. Meixner, and J. Williams
Biogeosciences Discuss., https://doi.org/10.5194/bgd-11-12009-2014, https://doi.org/10.5194/bgd-11-12009-2014, 2014
Revised manuscript not accepted
A. K. Mishra, K. Klingmueller, E. Fredj, J. Lelieveld, Y. Rudich, and I. Koren
Atmos. Chem. Phys., 14, 7213–7231, https://doi.org/10.5194/acp-14-7213-2014, https://doi.org/10.5194/acp-14-7213-2014, 2014
E. Bourtsoukidis, J. Williams, J. Kesselmeier, S. Jacobi, and B. Bonn
Atmos. Chem. Phys., 14, 6495–6510, https://doi.org/10.5194/acp-14-6495-2014, https://doi.org/10.5194/acp-14-6495-2014, 2014
T. Christoudias, Y. Proestos, and J. Lelieveld
Atmos. Chem. Phys., 14, 4607–4616, https://doi.org/10.5194/acp-14-4607-2014, https://doi.org/10.5194/acp-14-4607-2014, 2014
G. W. Mann, K. S. Carslaw, C. L. Reddington, K. J. Pringle, M. Schulz, A. Asmi, D. V. Spracklen, D. A. Ridley, M. T. Woodhouse, L. A. Lee, K. Zhang, S. J. Ghan, R. C. Easter, X. Liu, P. Stier, Y. H. Lee, P. J. Adams, H. Tost, J. Lelieveld, S. E. Bauer, K. Tsigaridis, T. P. C. van Noije, A. Strunk, E. Vignati, N. Bellouin, M. Dalvi, C. E. Johnson, T. Bergman, H. Kokkola, K. von Salzen, F. Yu, G. Luo, A. Petzold, J. Heintzenberg, A. Clarke, J. A. Ogren, J. Gras, U. Baltensperger, U. Kaminski, S. G. Jennings, C. D. O'Dowd, R. M. Harrison, D. C. S. Beddows, M. Kulmala, Y. Viisanen, V. Ulevicius, N. Mihalopoulos, V. Zdimal, M. Fiebig, H.-C. Hansson, E. Swietlicki, and J. S. Henzing
Atmos. Chem. Phys., 14, 4679–4713, https://doi.org/10.5194/acp-14-4679-2014, https://doi.org/10.5194/acp-14-4679-2014, 2014
W. Song, M. Staudt, I. Bourgeois, and J. Williams
Biogeosciences, 11, 1435–1447, https://doi.org/10.5194/bg-11-1435-2014, https://doi.org/10.5194/bg-11-1435-2014, 2014
J. A. Adame, M. Martínez, M. Sorribas, P. J. Hidalgo, H. Harder, J.-M. Diesch, F. Drewnick, W. Song, J. Williams, V. Sinha, M. A. Hernández-Ceballos, J. Vilà-Guerau de Arellano, R. Sander, Z. Hosaynali-Beygi, H. Fischer, J. Lelieveld, and B. De la Morena
Atmos. Chem. Phys., 14, 2325–2342, https://doi.org/10.5194/acp-14-2325-2014, https://doi.org/10.5194/acp-14-2325-2014, 2014
C. Liu, S. Beirle, T. Butler, P. Hoor, C. Frankenberg, P. Jöckel, M. Penning de Vries, U. Platt, A. Pozzer, M. G. Lawrence, J. Lelieveld, H. Tost, and T. Wagner
Atmos. Chem. Phys., 14, 1717–1732, https://doi.org/10.5194/acp-14-1717-2014, https://doi.org/10.5194/acp-14-1717-2014, 2014
Y. F. Elshorbany, P. J. Crutzen, B. Steil, A. Pozzer, H. Tost, and J. Lelieveld
Atmos. Chem. Phys., 14, 1167–1184, https://doi.org/10.5194/acp-14-1167-2014, https://doi.org/10.5194/acp-14-1167-2014, 2014
D. Giannadaki, A. Pozzer, and J. Lelieveld
Atmos. Chem. Phys., 14, 957–968, https://doi.org/10.5194/acp-14-957-2014, https://doi.org/10.5194/acp-14-957-2014, 2014
M. J. Tang, G. Schuster, and J. N. Crowley
Atmos. Chem. Phys., 14, 245–254, https://doi.org/10.5194/acp-14-245-2014, https://doi.org/10.5194/acp-14-245-2014, 2014
P. Zanis, P. Hadjinicolaou, A. Pozzer, E. Tyrlis, S. Dafka, N. Mihalopoulos, and J. Lelieveld
Atmos. Chem. Phys., 14, 115–132, https://doi.org/10.5194/acp-14-115-2014, https://doi.org/10.5194/acp-14-115-2014, 2014
A. L. Corrigan, L. M. Russell, S. Takahama, M. Äijälä, M. Ehn, H. Junninen, J. Rinne, T. Petäjä, M. Kulmala, A. L. Vogel, T. Hoffmann, C. J. Ebben, F. M. Geiger, P. Chhabra, J. H. Seinfeld, D. R. Worsnop, W. Song, J. Auld, and J. Williams
Atmos. Chem. Phys., 13, 12233–12256, https://doi.org/10.5194/acp-13-12233-2013, https://doi.org/10.5194/acp-13-12233-2013, 2013
J. Yoon, A. Pozzer, P. Hoor, D. Y. Chang, S. Beirle, T. Wagner, S. Schloegl, J. Lelieveld, and H. M. Worden
Atmos. Chem. Phys., 13, 11307–11316, https://doi.org/10.5194/acp-13-11307-2013, https://doi.org/10.5194/acp-13-11307-2013, 2013
A. L. Vogel, M. Äijälä, A. L. Corrigan, H. Junninen, M. Ehn, T. Petäjä, D. R. Worsnop, M. Kulmala, L. M. Russell, J. Williams, and T. Hoffmann
Atmos. Chem. Phys., 13, 10933–10950, https://doi.org/10.5194/acp-13-10933-2013, https://doi.org/10.5194/acp-13-10933-2013, 2013
E. Regelin, H. Harder, M. Martinez, D. Kubistin, C. Tatum Ernest, H. Bozem, T. Klippel, Z. Hosaynali-Beygi, H. Fischer, R. Sander, P. Jöckel, R. Königstedt, and J. Lelieveld
Atmos. Chem. Phys., 13, 10703–10720, https://doi.org/10.5194/acp-13-10703-2013, https://doi.org/10.5194/acp-13-10703-2013, 2013
M. Ammann, R. A. Cox, J. N. Crowley, M. E. Jenkin, A. Mellouki, M. J. Rossi, J. Troe, and T. J. Wallington
Atmos. Chem. Phys., 13, 8045–8228, https://doi.org/10.5194/acp-13-8045-2013, https://doi.org/10.5194/acp-13-8045-2013, 2013
J. Lelieveld, C. Barlas, D. Giannadaki, and A. Pozzer
Atmos. Chem. Phys., 13, 7023–7037, https://doi.org/10.5194/acp-13-7023-2013, https://doi.org/10.5194/acp-13-7023-2013, 2013
A.C. Nölscher, E. Bourtsoukidis, B. Bonn, J. Kesselmeier, J. Lelieveld, and J. Williams
Biogeosciences, 10, 4241–4257, https://doi.org/10.5194/bg-10-4241-2013, https://doi.org/10.5194/bg-10-4241-2013, 2013
M. D. Andrés-Hernández, D. Kartal, J. N. Crowley, V. Sinha, E. Regelin, M. Martínez-Harder, V. Nenakhov, J. Williams, H. Harder, H. Bozem, W. Song, J. Thieser, M. J. Tang, Z. Hosaynali Beigi, and J. P. Burrows
Atmos. Chem. Phys., 13, 5731–5749, https://doi.org/10.5194/acp-13-5731-2013, https://doi.org/10.5194/acp-13-5731-2013, 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
C. Brühl, J. Lelieveld, M. Höpfner, and H. Tost
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-13-11395-2013, https://doi.org/10.5194/acpd-13-11395-2013, 2013
Revised manuscript not accepted
A. L. Vogel, M. Äijälä, M. Brüggemann, M. Ehn, H. Junninen, T. Petäjä, D. R. Worsnop, M. Kulmala, J. Williams, and T. Hoffmann
Atmos. Meas. Tech., 6, 431–443, https://doi.org/10.5194/amt-6-431-2013, https://doi.org/10.5194/amt-6-431-2013, 2013
G. J. Phillips, U. Makkonen, G. Schuster, N. Sobanski, H. Hakola, and J. N. Crowley
Atmos. Meas. Tech., 6, 231–237, https://doi.org/10.5194/amt-6-231-2013, https://doi.org/10.5194/amt-6-231-2013, 2013
G. J. Phillips, N. Pouvesle, J. Thieser, G. Schuster, R. Axinte, H. Fischer, J. Williams, J. Lelieveld, and J. N. Crowley
Atmos. Chem. Phys., 13, 1129–1139, https://doi.org/10.5194/acp-13-1129-2013, https://doi.org/10.5194/acp-13-1129-2013, 2013
J. Lelieveld, M. G. Lawrence, and D. Kunkel
Atmos. Chem. Phys., 13, 31–34, https://doi.org/10.5194/acp-13-31-2013, https://doi.org/10.5194/acp-13-31-2013, 2013
A. Jugold, F. Althoff, M. Hurkuck, M. Greule, K. Lenhart, J. Lelieveld, and F. Keppler
Biogeosciences, 9, 5291–5301, https://doi.org/10.5194/bg-9-5291-2012, https://doi.org/10.5194/bg-9-5291-2012, 2012
A. C. Nölscher, V. Sinha, S. Bockisch, T. Klüpfel, and J. Williams
Atmos. Meas. Tech., 5, 2981–2992, https://doi.org/10.5194/amt-5-2981-2012, https://doi.org/10.5194/amt-5-2981-2012, 2012
Related subject area
Subject: Gases | Research Activity: Field Measurements | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Mechanistic insights into chloroacetic acid production from atmospheric multiphase volatile organic compound–chlorine chemistry
Accurate elucidation of oxidation under heavy ozone pollution: a full suite of radical measurements in the chemically complex atmosphere
Emissions of intermediate-volatility and semi-volatile organic compounds (I/SVOCs) from different cumulative-mileage diesel vehicles at various ambient temperatures
Characterization of nitrous acid and its potential effects on secondary pollution in the warm season in Beijing urban areas
Vertical changes in volatile organic compounds (VOCs) and impacts on photochemical ozone formation
Diurnal, seasonal, and interannual variations in δ(18O) of atmospheric O2 and its application to evaluate natural and anthropogenic changes in oxygen, carbon, and water cycles
Cloud processing of dimethyl sulfide (DMS) oxidation products limits sulfur dioxide (SO2) and carbonyl sulfide (OCS) production in the eastern North Atlantic marine boundary layer
Atmospheric carbonyl compounds are crucial in regional ozone heavy pollution: insights from the Chengdu Plain Urban Agglomeration, China
Understanding summertime peroxyacetyl nitrate (PAN) formation and its relation to aerosol pollution: insights from high-resolution measurements and modeling
Measurement report: Exploring the variations in ambient BTEX in urban Europe and their environmental health implications
Seasonal air concentration variability, gas–particle partitioning, precipitation scavenging, and air–water equilibrium of organophosphate esters in southern Canada
Measurement report: Surface exchange fluxes of HONO during the growth process of paddy fields in the Huaihe River Basin, China
Marine emissions and trade winds control the atmospheric nitrous oxide in the Galapagos Islands
Molecular and seasonal characteristics of organic vapors in urban Beijing: insights from Vocus-PTR measurements
The variations in volatile organic compounds based on the policy change for Omicron in the traffic hub of Zhengzhou
On the dynamics of ozone depletion events at Villum Research Station in the High Arctic
VOC sources and impacts at an urban Mediterranean area (Marseille – France)
Measurement report: Long-term measurements of surface ozone and trends in semi-natural sub-Saharan African ecosystems
Characterization of biogenic volatile organic compounds and their oxidation products in a stressed spruce-dominated forest close to a biogas power plant
Reactive chlorine-, sulfur-, and nitrogen-containing volatile organic compounds impact atmospheric chemistry in the megacity of Delhi during both clean and extremely polluted seasons
Analysis of the day-to-day variability of ozone vertical profiles in the lower troposphere during the 2022 Paris ACROSS campaign
Short lifetimes of organic nitrates in a sub-urban temperate forest indicate efficient assimilation of reactive nitrogen by the biosphere
Ozone deposition measurements over wheat fields in the North China Plain: variability and related factors of deposition flux and velocity
The impact of organic nitrates on summer ozone formation in Shanghai, China
Consistency evaluation of tropospheric ozone from ozonesonde and IAGOS (In-service Aircraft for a Global Observing System) observations: vertical distribution, ozonesonde types, and station–airport distance
CO2 and CO temporal variability over Mexico City from ground-based total column and surface measurements
Investigating carbonyl compounds above the Amazon rainforest using a proton-transfer-reaction time-of-flight mass spectrometer (PTR-ToF-MS) with NO+ chemical ionization
Measurement report: In-flight and ground-based measurements of nitrogen oxide emissions from latest-generation jet engines and 100 % sustainable aviation fuel
Differences in key volatile organic compound species in ozone formation between their initial and measured concentrations
Measurement report: Sources, sinks, and lifetime of NOx in a suburban temperate forest at night
Measurement report: Urban ammonia and amines in Houston, Texas
Biomass-burning sources control ambient particulate matter, but traffic and industrial sources control volatile organic compound (VOC) emissions and secondary-pollutant formation during extreme pollution events in Delhi
Multi-year observations of variable incomplete combustion in the New York megacity
Observations of the vertical distributions of summertime atmospheric pollutants in Nam Co: OH production and source analysis
Spatiotemporal variations in atmospheric CH4 concentrations and enhancements in northern China based on a comprehensive dataset: Ground-based observations, TROPOMI data, inventory data and inversions
Measurement report: Elevated atmospheric ammonia may promote particle pH and HONO formation – insights from the COVID-19 pandemic
Measurement report: Vertical and temporal variability in the near-surface ozone production rate and sensitivity in an urban area in the Pearl River Delta region, China
Elevated oxidized mercury in the free troposphere: analytical advances and application at a remote continental mountaintop site
Using observed urban NOx sinks to constrain VOC reactivity and the ozone and radical budget in the Seoul Metropolitan Area
Real-world emission characteristics of VOCs from typical cargo ships and their potential contributions to secondary organic aerosol and O3 under low-sulfur fuel policies
NO3 reactivity during a summer period in a temperate forest below and above the canopy
The role of oceanic ventilation and terrestrial outflow in atmospheric non-methane hydrocarbons over the Chinese marginal seas
Concentration and source changes of nitrous acid (HONO) during the COVID-19 lockdown in Beijing
Characteristics and sources of nonmethane volatile organic compounds (NMVOCs) and O3–NOx–NMVOC relationships in Zhengzhou, China
Measurement report: TURBAN observation campaign combining street-level low-cost air quality sensors and meteorological profile measurements in Prague
Deciphering anthropogenic and biogenic contributions to selected non-methane volatile organic compound emissions in an urban area
Emission characteristics of reactive organic gases (ROGs) from industrial volatile chemical products (VCPs) in the Pearl River Delta (PRD), China
Measurement report: Enhanced photochemical formation of formic and isocyanic acids in urban regions aloft – insights from tower-based online gradient measurements
Sources of organic gases and aerosol particles and their roles in nighttime particle growth at a rural forested site in southwest Germany
Surface snow bromide and nitrate at Eureka, Canada, in early spring and implications for polar boundary layer chemistry
Mingxue Li, Men Xia, Chunshui Lin, Yifan Jiang, Weihang Sun, Yurun Wang, Yingnan Zhang, Maoxia He, and Tao Wang
Atmos. Chem. Phys., 25, 3753–3764, https://doi.org/10.5194/acp-25-3753-2025, https://doi.org/10.5194/acp-25-3753-2025, 2025
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Our field campaigns observed a strong diel pattern of chloroacetic acid as well as a strong correlation between its level and that of reactive chlorine species at a coastal site. Using quantum chemical calculations and box model simulation with an updated Master Chemical Mechanism, we found that the formation pathway of chloroacetic acid involved multiphase processes. Our study enhances understanding of atmospheric organic chlorine chemistry and emphasizes the importance of multiphase reactions.
Renzhi Hu, Guoxian Zhang, Haotian Cai, Jingyi Guo, Keding Lu, Xin Li, Shengrong Lou, Zhaofeng Tan, Changjin Hu, Pinhua Xie, and Wenqing Liu
Atmos. Chem. Phys., 25, 3011–3028, https://doi.org/10.5194/acp-25-3011-2025, https://doi.org/10.5194/acp-25-3011-2025, 2025
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A full suite of radical measurements (OH, HO2, RO2, and kOH) was established to accurately elucidate the limitations of oxidation in a chemically complex atmosphere. Sensitivity tests revealed that the incorporation of complex processes enabled a balance in both radical concentrations and coordinate ratios, effectively addressing the deficiency in the ozone generation mechanism. The full-chain radical detection bridged the gap between the photochemistry and the intensive oxidation level.
Shuwen Guo, Xuan Zheng, Xiao He, Lewei Zeng, Liqiang He, Xian Wu, Yifei Dai, Zihao Huang, Ting Chen, Shupei Xiao, Yan You, Sheng Xiang, Shaojun Zhang, Jingkun Jiang, and Ye Wu
Atmos. Chem. Phys., 25, 2695–2705, https://doi.org/10.5194/acp-25-2695-2025, https://doi.org/10.5194/acp-25-2695-2025, 2025
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We considered two potential influencing factors of heavy-duty diesel vehicle emissions that are rarely mentioned in the literature: cumulative mileage and ambient temperatures. The results suggest that prolonged use of heavy-duty diesel vehicles and low ambient temperatures leads to reduced engine combustion efficiency, which in turn increases tailpipe emissions significantly.
Junling Li, Chaofan Lian, Mingyuan Liu, Hao Zhang, Yongxin Yan, Yufei Song, Chun Chen, Jiaqi Wang, Haijie Zhang, Yanqin Ren, Yucong Guo, Weigang Wang, Yisheng Xu, Hong Li, Jian Gao, and Maofa Ge
Atmos. Chem. Phys., 25, 2551–2568, https://doi.org/10.5194/acp-25-2551-2025, https://doi.org/10.5194/acp-25-2551-2025, 2025
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As a key source of hydroxyl (OH) radical, nitrous acid (HONO) has attracted much attention for its important role in the atmospheric oxidant capacity (AOC) increase. In this study, we made a comparison of the ambient levels, variation patterns, sources, and formation pathway in the warm season on the basis of continuous intensive observations at an urban site of Beijing. This work highlights the importance of HONO for the AOC in the warm season.
Xiao-Bing Li, Bin Yuan, Yibo Huangfu, Suxia Yang, Xin Song, Jipeng Qi, Xianjun He, Sihang Wang, Yubin Chen, Qing Yang, Yongxin Song, Yuwen Peng, Guiqian Tang, Jian Gao, Dasa Gu, and Min Shao
Atmos. Chem. Phys., 25, 2459–2472, https://doi.org/10.5194/acp-25-2459-2025, https://doi.org/10.5194/acp-25-2459-2025, 2025
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Online vertical gradient measurements of volatile organic compounds (VOCs), ozone, and NOx were conducted based on a 325 m tall tower in urban Beijing. Vertical changes in the concentrations, compositions, key drivers, and environmental impacts of VOCs were analyzed in this study. We find that VOC species display differentiated vertical variation patterns and distinct roles in contributing to photochemical ozone formation with increasing height in the urban planetary boundary layer.
Shigeyuki Ishidoya, Satoshi Sugawara, and Atsushi Okazaki
Atmos. Chem. Phys., 25, 1965–1987, https://doi.org/10.5194/acp-25-1965-2025, https://doi.org/10.5194/acp-25-1965-2025, 2025
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The 18O/16O ratio of atmospheric oxygen, δatm(18O), is higher than that of ocean water due to isotopic effects during biospheric activities. This is known as the Dole–Morita effect, and its millennial-scale variations are recorded in ice cores. However, small variations of δatm(18O) in the present day have never been detected so far. This paper presents the first observations of diurnal, seasonal, and secular variations in δatm(18O) and applies them to evaluate oxygen, carbon, and water cycles.
Delaney B. Kilgour, Christopher M. Jernigan, Olga Garmash, Sneha Aggarwal, Shengqian Zhou, Claudia Mohr, Matt E. Salter, Joel A. Thornton, Jian Wang, Paul Zieger, and Timothy H. Bertram
Atmos. Chem. Phys., 25, 1931–1947, https://doi.org/10.5194/acp-25-1931-2025, https://doi.org/10.5194/acp-25-1931-2025, 2025
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We report simultaneous measurements of dimethyl sulfide (DMS) and hydroperoxymethyl thioformate (HPMTF) in the eastern North Atlantic. We use an observationally constrained box model to show that cloud loss is the dominant sink of HPMTF in this region over 6 weeks, resulting in large reductions in DMS-derived products that contribute to aerosol formation and growth. Our findings indicate that fast cloud processing of HPMTF must be included in global models to accurately capture the sulfur cycle.
Jiemeng Bao, Xin Zhang, Zhenhai Wu, Li Zhou, Jun Qian, Qinwen Tan, Fumo Yang, Junhui Chen, Yunfeng Li, Hefan Liu, Liqun Deng, and Hong Li
Atmos. Chem. Phys., 25, 1899–1916, https://doi.org/10.5194/acp-25-1899-2025, https://doi.org/10.5194/acp-25-1899-2025, 2025
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We studied carbonyl compounds' role in ozone pollution in the Chengdu Plain Urban Agglomeration, China. During heavy pollution in August 2019, we measured carbonyls at nine sites and analyzed their impact. Areas with higher carbonyl levels, like Chengdu, had worse ozone pollution. While their abundance matters, chemical reactions with other pollutants are the main drivers. Our findings show regional cooperation is vital to reducing ozone pollution effectively.
Baoye Hu, Naihua Chen, Rui Li, Mingqiang Huang, Jinsheng Chen, Youwei Hong, Lingling Xu, Xiaolong Fan, Mengren Li, Lei Tong, Qiuping Zheng, and Yuxiang Yang
Atmos. Chem. Phys., 25, 905–921, https://doi.org/10.5194/acp-25-905-2025, https://doi.org/10.5194/acp-25-905-2025, 2025
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Box modeling with the Master Chemical Mechanism (MCM) was used to explore summertime peroxyacetyl nitrate (PAN) formation and its link to aerosol pollution under high-ozone conditions. The MCM model is effective in the study of PAN photochemical formation and performed better during the clean period than the haze period. Machine learning analysis identified ammonia, nitrate, and fine particulate matter as the top three factors contributing to simulation bias.
Xiansheng Liu, Xun Zhang, Marvin Dufresne, Tao Wang, Lijie Wu, Rosa Lara, Roger Seco, Marta Monge, Ana Maria Yáñez-Serrano, Marie Gohy, Paul Petit, Audrey Chevalier, Marie-Pierre Vagnot, Yann Fortier, Alexia Baudic, Véronique Ghersi, Grégory Gille, Ludovic Lanzi, Valérie Gros, Leïla Simon, Heidi Héllen, Stefan Reimann, Zoé Le Bras, Michelle Jessy Müller, David Beddows, Siqi Hou, Zongbo Shi, Roy M. Harrison, William Bloss, James Dernie, Stéphane Sauvage, Philip K. Hopke, Xiaoli Duan, Taicheng An, Alastair C. Lewis, James R. Hopkins, Eleni Liakakou, Nikolaos Mihalopoulos, Xiaohu Zhang, Andrés Alastuey, Xavier Querol, and Thérèse Salameh
Atmos. Chem. Phys., 25, 625–638, https://doi.org/10.5194/acp-25-625-2025, https://doi.org/10.5194/acp-25-625-2025, 2025
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This study examines BTEX (benzene, toluene, ethylbenzene, xylenes) pollution in urban areas across seven European countries. Analyzing data from 22 monitoring sites, we found traffic and industrial activities significantly impact BTEX levels, with peaks during rush hours. The risk from BTEX exposure remains moderate, especially in high-traffic and industrial zones, highlighting the need for targeted air quality management to protect public health and improve urban air quality.
Yuening Li, Faqiang Zhan, Chubashini Shunthirasingham, Ying Duan Lei, Jenny Oh, Amina Ben Chaaben, Zhe Lu, Kelsey Lee, Frank A. P. C. Gobas, Hayley Hung, and Frank Wania
Atmos. Chem. Phys., 25, 459–472, https://doi.org/10.5194/acp-25-459-2025, https://doi.org/10.5194/acp-25-459-2025, 2025
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Organophosphate esters are important humanmade trace contaminants. Measuring them in the atmospheric gas phase, particles, precipitation, and surface water in Canada, we explore seasonal concentration variability, gas–particle partitioning, precipitation scavenging, and the air–water equilibrium. Whereas higher summer concentrations and efficient precipitation scavenging conform with expectations, the lack of a relationship between compound volatility and gas–particle partitioning is puzzling.
Fanhao Meng, Baobin Han, Min Qin, Wu Fang, Ke Tang, Dou Shao, Zhitang Liao, Jun Duan, Yan Feng, Yong Huang, Ting Ni, and Pinhua Xie
Atmos. Chem. Phys., 24, 14191–14208, https://doi.org/10.5194/acp-24-14191-2024, https://doi.org/10.5194/acp-24-14191-2024, 2024
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Comprehensive observations of HONO and NOx fluxes were conducted over paddy fields in the Huaihe River Basin. Consecutive peaks in HONO and NO fluxes suggest a potentially enhanced release of HONO and NO due to soil tillage, whereas waterlogged soil may inhibit microbial nitrification processes following irrigation. Notably, biological processes and light-driven NO2 reactions at the surface may serve as sources of HONO and influence the local HONO budget during rotary tillage.
Timur Cinay, Dickon Young, Nazaret Narváez Jimenez, Cristina Vintimilla-Palacios, Ariel Pila Alonso, Paul B. Krummel, William Vizuete, and Andrew R. Babbin
EGUsphere, https://doi.org/10.5194/egusphere-2024-3769, https://doi.org/10.5194/egusphere-2024-3769, 2024
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We present the initial 15 months of nitrous oxide measurements from the Galapagos Emissions Monitoring Station. The observed variability in atmospheric mole fractions during this period can be linked to several factors: seasonal variations in trade wind speed and direction across the eastern Pacific, differences in the transport history of air masses sampled, and spatiotemporal heterogeneity in regional marine nitrous oxide emissions from coastal upwelling systems of Peru and Chile.
Zhaojin An, Rujing Yin, Xinyan Zhao, Xiaoxiao Li, Yuyang Li, Yi Yuan, Junchen Guo, Yiqi Zhao, Xue Li, Dandan Li, Yaowei Li, Dongbin Wang, Chao Yan, Kebin He, Douglas R. Worsnop, Frank N. Keutsch, and Jingkun Jiang
Atmos. Chem. Phys., 24, 13793–13810, https://doi.org/10.5194/acp-24-13793-2024, https://doi.org/10.5194/acp-24-13793-2024, 2024
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Online Vocus-PTR measurements show the compositions and seasonal variations in organic vapors in urban Beijing. With enhanced sensitivity and mass resolution, various species at a level of sub-parts per trillion (ppt) and organics with multiple oxygens (≥ 3) were observed. The fast photooxidation process in summer leads to an increase in both concentration and proportion of organics with multiple oxygens, while, in other seasons, the variations in them could be influenced by mixed sources.
Bowen Zhang, Dong Zhang, Zhe Dong, Xinshuai Song, Ruiqin Zhang, and Xiao Li
Atmos. Chem. Phys., 24, 13587–13601, https://doi.org/10.5194/acp-24-13587-2024, https://doi.org/10.5194/acp-24-13587-2024, 2024
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To gain insight into the impact of changes due to epidemic control policies, we undertook continuous online monitoring of volatile organic compounds (VOCs) at an urban site in Zhengzhou over a 2-month period. This study examines the characteristics of VOCs, their sources, and their temporal evolution. It also assesses the impact of the policy change on VOC pollution during the monitoring period, thus providing a basis for further research on VOC pollution and source control.
Jakob Boyd Pernov, Jens Liengaard Hjorth, Lise Lotte Sørensen, and Henrik Skov
Atmos. Chem. Phys., 24, 13603–13631, https://doi.org/10.5194/acp-24-13603-2024, https://doi.org/10.5194/acp-24-13603-2024, 2024
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Arctic ozone depletion events (ODEs) occur every spring and have vast implications for the oxidizing capacity, radiative balance, and mercury oxidation. In this study, we analyze ozone, ODEs, and their connection to meteorological and air mass history variables through statistical analyses, back trajectories, and machine learning (ML) at Villum Research Station. ODEs are favorable under sunny, calm conditions with air masses arriving from northerly wind directions with sea ice contact.
Marvin Dufresne, Thérèse Salameh, Thierry Léonardis, Grégory Gille, Alexandre Armengaud, and Stéphane Sauvage
EGUsphere, https://doi.org/10.5194/egusphere-2024-3576, https://doi.org/10.5194/egusphere-2024-3576, 2024
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This paper is about the eighteen-months measurement of Non-Methane Hydrocarbons (NMHC) at Marseille, were there was no measurement since early 2000 despite the impact of NMHC on air quality and climate. The traffic related sources are the first contributor to NMHC concentrations in Marseille and shipping strongly contribute to the formation of aerosols. Finally, the lockdown due to the Covid-19 had an impact on NMHC concentrations reaching a fifty percents decreasing for traffic-related sources.
Hagninou Elagnon Venance Donnou, Aristide Barthélémy Akpo, Money Ossohou, Claire Delon, Véronique Yoboué, Dungall Laouali, Marie Ouafo-Leumbe, Pieter Gideon Van Zyl, Ousmane Ndiaye, Eric Gardrat, Maria Dias-Alves, and Corinne Galy-Lacaux
Atmos. Chem. Phys., 24, 13151–13182, https://doi.org/10.5194/acp-24-13151-2024, https://doi.org/10.5194/acp-24-13151-2024, 2024
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Ozone is a secondary air pollutant that is detrimental to human and plant health. A better understanding of its chemical evolution is a challenge for Africa, where it is still undersampled. Out of 14 sites examined (1995–2020), high levels of O3 are reported in southern Africa. The dominant chemical processes leading to O3 formation are identified. A decrease in O3 is observed at Katibougou (Mali) and Banizoumbou (Niger), and an increase is found at Zoétélé (Cameroon) and Skukuza (South Africa).
Junwei Song, Georgios I. Gkatzelis, Ralf Tillmann, Nicolas Brüggemann, Thomas Leisner, and Harald Saathoff
Atmos. Chem. Phys., 24, 13199–13217, https://doi.org/10.5194/acp-24-13199-2024, https://doi.org/10.5194/acp-24-13199-2024, 2024
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Biogenic volatile organic compounds (BVOCs) and organic aerosol (OA) particles were measured online in a stressed spruce-dominated forest. OA was mainly attributed to the monoterpene oxidation products. The mixing ratios of BVOCs were higher than the values previously measured in other temperate forests. The results demonstrate that BVOCs are influenced not only by meteorology and biogenic emissions but also by local anthropogenic emissions and subsequent chemical transformation processes.
Sachin Mishra, Vinayak Sinha, Haseeb Hakkim, Arpit Awasthi, Sachin D. Ghude, Vijay Kumar Soni, Narendra Nigam, Baerbel Sinha, and Madhavan N. Rajeevan
Atmos. Chem. Phys., 24, 13129–13150, https://doi.org/10.5194/acp-24-13129-2024, https://doi.org/10.5194/acp-24-13129-2024, 2024
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We quantified 111 gases using mass spectrometry to understand how seasonal and emission changes lead from clean air in the monsoon season to extremely polluted air in the post-monsoon season in Delhi. Averaged total mass concentrations (260 µg m-3) were > 4 times in polluted periods, driven by biomass burning emissions and reduced atmospheric ventilation. Reactive gaseous nitrogen, chlorine, and sulfur compounds hitherto unreported from such a polluted environment were discovered.
Gérard Ancellet, Camille Viatte, Anne Boynard, François Ravetta, Jacques Pelon, Cristelle Cailteau-Fischbach, Pascal Genau, Julie Capo, Axel Roy, and Philippe Nédélec
Atmos. Chem. Phys., 24, 12963–12983, https://doi.org/10.5194/acp-24-12963-2024, https://doi.org/10.5194/acp-24-12963-2024, 2024
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Characterization of ozone pollution in urban areas benefited from a measurement campaign in summer 2022 in the Paris region. The analysis is based on 21 d of lidar and aircraft observations. The main objective is an analysis of the sensitivity of ozone pollution to the micrometeorological processes in the urban atmospheric boundary layer and the transport of regional pollution. The paper also discusses to what extent satellite observations can track observed ozone plumes.
Simone T. Andersen, Rolf Sander, Patrick Dewald, Laura Wüst, Tobias Seubert, Gunther N. T. E. Türk, Jan Schuladen, Max R. McGillen, Chaoyang Xue, Abdelwahid Mellouki, Alexandre Kukui, Vincent Michoud, Manuela Cirtog, Mathieu Cazaunau, Astrid Bauville, Hichem Bouzidi, Paola Formenti, Cyrielle Denjean, Jean-Claude Etienne, Olivier Garrouste, Christopher Cantrell, Jos Lelieveld, and John N. Crowley
EGUsphere, https://doi.org/10.5194/egusphere-2024-3437, https://doi.org/10.5194/egusphere-2024-3437, 2024
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Measurements and modelling of reactive nitrogen gases observed in a suburban temperate forest in Rambouillet, France circa 50 km southwest of Paris in 2022 indicate that the biosphere rapidly scavenges organic nitrates of mixed biogenic and anthropogenic origin, resulting in short lifetimes for e.g. alkyl nitrates and peroxy nitrates.
Xiaoyi Zhang, Wanyun Xu, Weili Lin, Gen Zhang, Jinjian Geng, Li Zhou, Huarong Zhao, Sanxue Ren, Guangsheng Zhou, Jianmin Chen, and Xiaobin Xu
Atmos. Chem. Phys., 24, 12323–12340, https://doi.org/10.5194/acp-24-12323-2024, https://doi.org/10.5194/acp-24-12323-2024, 2024
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Ozone (O3) deposition is a key process that removes surface O3, affecting air quality, ecosystems and climate change. We conducted O3 deposition measurement over a wheat canopy using a newly relaxed eddy accumulation flux system. Large variabilities in O3 deposition were detected, mainly determined by crop growth and modulated by various environmental factors. More O3 deposition observations over different surfaces are needed for exploring deposition mechanisms and model optimization.
Chunmeng Li, Xiaorui Chen, Haichao Wang, Tianyu Zhai, Xuefei Ma, Xinping Yang, Shiyi Chen, Min Zhou, Shengrong Lou, Xin Li, Limin Zeng, and Keding Lu
EGUsphere, https://doi.org/10.5194/egusphere-2024-3337, https://doi.org/10.5194/egusphere-2024-3337, 2024
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This study reports an observation of organic nitrate (including total peroxy nitrates and total alkyl nitrates) in Shanghai, China during the summer of 2021, by a homemade thermal dissociation cavity-enhanced absorption spectrometer (TD-CEAS, Atmos. Meas. Tech., 14, 4033–4051, 2021). The distribution of organic nitrates and their effects on local ozone production are analyzed based on the field observation in conjunction with model simulation.
Honglei Wang, David W. Tarasick, Jane Liu, Herman G. J. Smit, Roeland Van Malderen, Lijuan Shen, Romain Blot, and Tianliang Zhao
Atmos. Chem. Phys., 24, 11927–11942, https://doi.org/10.5194/acp-24-11927-2024, https://doi.org/10.5194/acp-24-11927-2024, 2024
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In this study, we identify 23 suitable pairs of sites from World Ozone and Ultraviolet Radiation Data Centre (WOUDC) and In-service Aircraft for a Global Observing System (IAGOS) datasets (1995 to 2021), compare the average vertical distributions of tropospheric O3 from ozonesonde and aircraft measurements, and analyze the differences based on ozonesonde type and station–airport distance.
Noémie Taquet, Wolfgang Stremme, María Eugenia González del Castillo, Victor Almanza, Alejandro Bezanilla, Olivier Laurent, Carlos Alberti, Frank Hase, Michel Ramonet, Thomas Lauvaux, Ke Che, and Michel Grutter
Atmos. Chem. Phys., 24, 11823–11848, https://doi.org/10.5194/acp-24-11823-2024, https://doi.org/10.5194/acp-24-11823-2024, 2024
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We characterize the variability in CO and CO2 emissions over Mexico City from long-term time-resolved Fourier transform infrared spectroscopy solar absorption and surface measurements from 2013 to 2021. Using the average intraday CO growth rate from total columns, the average CO / CO2 ratio and TROPOMI data, we estimate the interannual variability in the CO and CO2 anthropogenic emissions of Mexico City, highlighting the effect of an unprecedented drop in activity due to the COVID-19 lockdown.
Akima Ringsdorf, Achim Edtbauer, Bruna Holanda, Christopher Poehlker, Marta O. Sá, Alessandro Araújo, Jürgen Kesselmeier, Jos Lelieveld, and Jonathan Williams
Atmos. Chem. Phys., 24, 11883–11910, https://doi.org/10.5194/acp-24-11883-2024, https://doi.org/10.5194/acp-24-11883-2024, 2024
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We show the average height distribution of separately observed aldehydes and ketones over a day and discuss their rainforest-specific sources and sinks as well as their seasonal changes above the Amazon. Ketones have much longer atmospheric lifetimes than aldehydes and thus different implications for atmospheric chemistry. However, they are commonly observed together, which we overcome by measuring with a NO+ chemical ionization mass spectrometer for the first time in the Amazon rainforest.
Theresa Harlass, Rebecca Dischl, Stefan Kaufmann, Raphael Märkl, Daniel Sauer, Monika Scheibe, Paul Stock, Tiziana Bräuer, Andreas Dörnbrack, Anke Roiger, Hans Schlager, Ulrich Schumann, Magdalena Pühl, Tobias Schripp, Tobias Grein, Linda Bondorf, Charles Renard, Maxime Gauthier, Mark Johnson, Darren Luff, Paul Madden, Peter Swann, Denise Ahrens, Reetu Sallinen, and Christiane Voigt
Atmos. Chem. Phys., 24, 11807–11822, https://doi.org/10.5194/acp-24-11807-2024, https://doi.org/10.5194/acp-24-11807-2024, 2024
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Emissions from aircraft have a direct impact on our climate. Here, we present airborne and ground-based measurement data of nitrogen oxides that were collected in the exhaust of an Airbus aircraft. We study the impact of burning fossil and sustainable aviation fuel on nitrogen oxide emissions at different engine settings related to combustor temperature, pressure and fuel flow. Further, we compare observations with engine emission models.
Xudong Zheng and Shaodong Xie
EGUsphere, https://doi.org/10.5194/egusphere-2024-2568, https://doi.org/10.5194/egusphere-2024-2568, 2024
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To reduce uncertainties in identifying key volatile organic compounds (VOCs) affecting ozone (O3) formation, this study focused on identifying key species based on initial VOC concentrations. Using reaction rates and observed VOCs concentrations, we calculated initial VOCs concentrations during the day and the night. Initial concentrations of alkenes and aromatics were higher than observed ones. Conversely, initial oxygenated VOC concentrations were lower than observed concentrations.
Simone T. Andersen, Max R. McGillen, Chaoyang Xue, Tobias Seubert, Patrick Dewald, Gunther N. T. E. Türk, Jan Schuladen, Cyrielle Denjean, Jean-Claude Etienne, Olivier Garrouste, Marina Jamar, Sergio Harb, Manuela Cirtog, Vincent Michoud, Mathieu Cazaunau, Antonin Bergé, Christopher Cantrell, Sebastien Dusanter, Bénédicte Picquet-Varrault, Alexandre Kukui, Abdelwahid Mellouki, Lucy J. Carpenter, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 24, 11603–11618, https://doi.org/10.5194/acp-24-11603-2024, https://doi.org/10.5194/acp-24-11603-2024, 2024
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Using measurements of various trace gases in a suburban forest near Paris in the summer of 2022, we were able to gain insight into the sources and sinks of NOx (NO+NO2) with a special focus on their nighttime chemical and physical loss processes. NO was observed as a result of nighttime soil emissions when O3 levels were strongly depleted by deposition. NO oxidation products were not observed at night, indicating that soil and/or foliar surfaces are an efficient sink of reactive N.
Lee Tiszenkel, James H. Flynn, and Shan-Hu Lee
Atmos. Chem. Phys., 24, 11351–11363, https://doi.org/10.5194/acp-24-11351-2024, https://doi.org/10.5194/acp-24-11351-2024, 2024
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Ammonia and amines are important ingredients for aerosol formation in urban environments, but the measurements of these compounds are extremely challenging. Our observations show that urban ammonia and amines in Houston are emitted from urban sources, and diurnal variations in their concentrations are likely governed by gas-to-particle conversion and emissions.
Arpit Awasthi, Baerbel Sinha, Haseeb Hakkim, Sachin Mishra, Varkrishna Mummidivarapu, Gurmanjot Singh, Sachin D. Ghude, Vijay Kumar Soni, Narendra Nigam, Vinayak Sinha, and Madhavan N. Rajeevan
Atmos. Chem. Phys., 24, 10279–10304, https://doi.org/10.5194/acp-24-10279-2024, https://doi.org/10.5194/acp-24-10279-2024, 2024
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We use 111 volatile organic compounds (VOCs), PM10, and PM2.5 in a positive matrix factorization (PMF) model to resolve 11 pollution sources validated with chemical fingerprints. Crop residue burning and heating account for ~ 50 % of the PM, while traffic and industrial emissions dominate the gas-phase VOC burden and formation potential of secondary organic aerosols (> 60 %). Non-tailpipe emissions from compressed-natural-gas-fuelled commercial vehicles dominate the transport sector's PM burden.
Luke D. Schiferl, Cong Cao, Bronte Dalton, Andrew Hallward-Driemeier, Ricardo Toledo-Crow, and Róisín Commane
Atmos. Chem. Phys., 24, 10129–10142, https://doi.org/10.5194/acp-24-10129-2024, https://doi.org/10.5194/acp-24-10129-2024, 2024
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Carbon monoxide (CO) is an air pollutant and an important indicator of the incomplete combustion of fossil fuels in cities. Using 4 years of winter and spring observations in New York City, we found that both the magnitude and variability of CO from the metropolitan area are greater than expected. Transportation emissions cannot explain the missing and variable CO, which points to energy from buildings as a likely underappreciated source of urban air pollution and greenhouse gas emissions.
Chengzhi Xing, Cheng Liu, Chunxiang Ye, Jingkai Xue, Hongyu Wu, Xiangguang Ji, Jinping Ou, and Qihou Hu
Atmos. Chem. Phys., 24, 10093–10112, https://doi.org/10.5194/acp-24-10093-2024, https://doi.org/10.5194/acp-24-10093-2024, 2024
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We identified the contributions of ozone (O3) and nitrous acid (HONO) to the production rates of hydroxide (OH) in vertical space on the Tibetan Plateau (TP). A new insight was offered: the contributions of HONO and O3 to the production rates of OH on the TP are even greater than in lower-altitudes areas. This study enriches the understanding of vertical distribution of atmospheric components and explains the strong atmospheric oxidation capacity (AOC) on the TP.
Pengfei Han, Ning Zeng, Bo Yao, Wen Zhang, Weijun Quan, Pucai Wang, Ting Wang, Minqiang Zhou, Qixiang Cai, Yuzhong Zhang, Ruosi Liang, Wanqi Sun, and Shengxiang Liu
EGUsphere, https://doi.org/10.5194/egusphere-2024-2162, https://doi.org/10.5194/egusphere-2024-2162, 2024
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Methane (CH4) is a potent greenhouse gas. Northern China contributes a large proportion of CH4 emissions yet large observation gaps are existed. Here we compiled a comprehensive dataset which is publicly available including ground-based, satellite-based, inventory and modeling results, to show the CH4 concentrations, enhancements and spatial-temporal variations. The data can benefit the research community, and policy makers for future observations, atmospheric inversions and policy-making.
Xinyuan Zhang, Lingling Wang, Nan Wang, Shuangliang Ma, Shenbo Wang, Ruiqin Zhang, Dong Zhang, Mingkai Wang, and Hongyu Zhang
Atmos. Chem. Phys., 24, 9885–9898, https://doi.org/10.5194/acp-24-9885-2024, https://doi.org/10.5194/acp-24-9885-2024, 2024
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This study highlights the importance of the redox reaction of NO2 with SO2 based on actual atmospheric observations. The particle pH in future China is expected to rise steadily. Consequently, this reaction could become a significant source of HONO in China. Therefore, it is crucial to coordinate the control of SO2, NOx, and NH3 emissions to avoid a rapid increase in the particle pH.
Jun Zhou, Chunsheng Zhang, Aiming Liu, Bin Yuan, Yan Wang, Wenjie Wang, Jie-Ping Zhou, Yixin Hao, Xiao-Bing Li, Xianjun He, Xin Song, Yubin Chen, Suxia Yang, Shuchun Yang, Yanfeng Wu, Bin Jiang, Shan Huang, Junwen Liu, Yuwen Peng, Jipeng Qi, Minhui Deng, Bowen Zhong, Yibo Huangfu, and Min Shao
Atmos. Chem. Phys., 24, 9805–9826, https://doi.org/10.5194/acp-24-9805-2024, https://doi.org/10.5194/acp-24-9805-2024, 2024
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In-depth understanding of the near-ground vertical variability in photochemical ozone (O3) formation is crucial for mitigating O3 pollution. Utilizing a self-built vertical observation system, a direct net photochemical O3 production rate detection system, and an observation-based model, we diagnosed the vertical distributions and formation mechanism of net photochemical O3 production rates and sensitivity in the Pearl River Delta region, one of the most O3-polluted areas in China.
Eleanor J. Derry, Tyler R. Elgiar, Taylor Y. Wilmot, Nicholas W. Hoch, Noah S. Hirshorn, Peter Weiss-Penzias, Christopher F. Lee, John C. Lin, A. Gannet Hallar, Rainer Volkamer, Seth N. Lyman, and Lynne E. Gratz
Atmos. Chem. Phys., 24, 9615–9643, https://doi.org/10.5194/acp-24-9615-2024, https://doi.org/10.5194/acp-24-9615-2024, 2024
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Mercury (Hg) is a globally distributed neurotoxic pollutant. Atmospheric deposition is the main source of Hg in ecosystems. However, measurement biases hinder understanding of the origins and abundance of the more bioavailable oxidized form. We used an improved, calibrated measurement system to study air mass composition and transport of atmospheric Hg at a remote mountaintop site in the central US. Oxidized Hg originated upwind in the low to middle free troposphere under clean, dry conditions.
Benjamin A. Nault, Katherine R. Travis, James H. Crawford, Donald R. Blake, Pedro Campuzano-Jost, Ronald C. Cohen, Joshua P. DiGangi, Glenn S. Diskin, Samuel R. Hall, L. Gregory Huey, Jose L. Jimenez, Kyung-Eun Min, Young Ro Lee, Isobel J. Simpson, Kirk Ullmann, and Armin Wisthaler
Atmos. Chem. Phys., 24, 9573–9595, https://doi.org/10.5194/acp-24-9573-2024, https://doi.org/10.5194/acp-24-9573-2024, 2024
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Ozone (O3) is a pollutant formed from the reactions of gases emitted from various sources. In urban areas, the density of human activities can increase the O3 formation rate (P(O3)), thus impacting air quality and health. Observations collected over Seoul, South Korea, are used to constrain P(O3). A high local P(O3) was found; however, local P(O3) was partly reduced due to compounds typically ignored. These observations also provide constraints for unmeasured compounds that will impact P(O3).
Fan Zhang, Binyu Xiao, Zeyu Liu, Yan Zhang, Chongguo Tian, Rui Li, Can Wu, Yali Lei, Si Zhang, Xinyi Wan, Yubao Chen, Yong Han, Min Cui, Cheng Huang, Hongli Wang, Yingjun Chen, and Gehui Wang
Atmos. Chem. Phys., 24, 8999–9017, https://doi.org/10.5194/acp-24-8999-2024, https://doi.org/10.5194/acp-24-8999-2024, 2024
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Mandatory use of low-sulfur fuel due to global sulfur limit regulations means large uncertainties in volatile organic compound (VOC) emissions. On-board tests of VOCs from nine cargo ships in China were carried out. Results showed that switching from heavy-fuel oil to diesel increased emission factor VOCs by 48 % on average, enhancing O3 and the secondary organic aerosol formation potential. Thus, implementing a global ultra-low-sulfur oil policy needs to be optimized in the near future.
Patrick Dewald, Tobias Seubert, Simone T. Andersen, Gunther N. T. E. Türk, Jan Schuladen, Max R. McGillen, Cyrielle Denjean, Jean-Claude Etienne, Olivier Garrouste, Marina Jamar, Sergio Harb, Manuela Cirtog, Vincent Michoud, Mathieu Cazaunau, Antonin Bergé, Christopher Cantrell, Sebastien Dusanter, Bénédicte Picquet-Varrault, Alexandre Kukui, Chaoyang Xue, Abdelwahid Mellouki, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 24, 8983–8997, https://doi.org/10.5194/acp-24-8983-2024, https://doi.org/10.5194/acp-24-8983-2024, 2024
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In the scope of a field campaign in a suburban forest near Paris in the summer of 2022, we measured the reactivity of the nitrate radical NO3 towards biogenic volatile organic compounds (BVOCs; e.g. monoterpenes) mainly below but also above the canopy. NO3 reactivity was the highest during nights with strong temperature inversions and decreased strongly with height. Reactions with BVOCs were the main removal process of NO3 throughout the diel cycle below the canopy.
Jian Wang, Lei Xue, Qianyao Ma, Feng Xu, Gaobin Xu, Shibo Yan, Jiawei Zhang, Jianlong Li, Honghai Zhang, Guiling Zhang, and Zhaohui Chen
Atmos. Chem. Phys., 24, 8721–8736, https://doi.org/10.5194/acp-24-8721-2024, https://doi.org/10.5194/acp-24-8721-2024, 2024
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This study investigated the distribution and sources of non-methane hydrocarbons (NMHCs) in the lower atmosphere over the marginal seas of China. NMHCs, a subset of volatile organic compounds (VOCs), play a crucial role in atmospheric chemistry. Derived from systematic atmospheric sampling in coastal cities and marginal sea regions, this study offers valuable insights into the interaction between land and sea in shaping offshore atmospheric NMHCs.
Yusheng Zhang, Feixue Zheng, Zemin Feng, Chaofan Lian, Weigang Wang, Xiaolong Fan, Wei Ma, Zhuohui Lin, Chang Li, Gen Zhang, Chao Yan, Ying Zhang, Veli-Matti Kerminen, Federico Bianch, Tuukka Petäjä, Juha Kangasluoma, Markku Kulmala, and Yongchun Liu
Atmos. Chem. Phys., 24, 8569–8587, https://doi.org/10.5194/acp-24-8569-2024, https://doi.org/10.5194/acp-24-8569-2024, 2024
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The nitrous acid (HONO) budget was validated during a COVID-19 lockdown event. The main conclusions are (1) HONO concentrations showed a significant decrease from 0.97 to 0.53 ppb during lockdown; (2) vehicle emissions accounted for 53 % of nighttime sources, with the heterogeneous conversion of NO2 on ground surfaces more important than aerosol; and (3) the dominant daytime source shifted from the homogenous reaction between NO and OH (51 %) to nitrate photolysis (53 %) during lockdown.
Dong Zhang, Xiao Li, Minghao Yuan, Yifei Xu, Qixiang Xu, Fangcheng Su, Shenbo Wang, and Ruiqin Zhang
Atmos. Chem. Phys., 24, 8549–8567, https://doi.org/10.5194/acp-24-8549-2024, https://doi.org/10.5194/acp-24-8549-2024, 2024
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The increasing concentration of O3 precursors and unfavorable meteorological conditions are key factors in the formation of O3 pollution in Zhengzhou. Vehicular exhausts (28 %), solvent usage (27 %), and industrial production (22 %) are identified as the main sources of NMVOCs. Moreover, O3 formation in Zhengzhou is found to be in an anthropogenic volatile organic compound (AVOC)-limited regime. Thus, to reduce O3 formation, a minimum AVOCs / NOx reduction ratio ≥ 3 : 1 is recommended.
Petra Bauerová, Josef Keder, Adriana Šindelářová, Ondřej Vlček, William Patiño, Jaroslav Resler, Pavel Krč, Jan Geletič, Hynek Řezníček, Martin Bureš, Kryštof Eben, Michal Belda, Jelena Radović, Vladimír Fuka, Radek Jareš, and Igor Ezau
EGUsphere, https://doi.org/10.5194/egusphere-2024-1222, https://doi.org/10.5194/egusphere-2024-1222, 2024
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We implemented an observation campaign focused on street-level air quality and vertical meteorological profile measurement in Prague using low-cost sensors and remote sensing devices. Low-cost sensors have undergone long-term field testing, own data correction and drift evaluation procedures. A high level of NO2 pollution was confirmed due to the traffic load in streets, peaks of aerosol pollution appeared more under inversion conditions. The data will be further used for PALM model validation.
Arianna Peron, Martin Graus, Marcus Striednig, Christian Lamprecht, Georg Wohlfahrt, and Thomas Karl
Atmos. Chem. Phys., 24, 7063–7083, https://doi.org/10.5194/acp-24-7063-2024, https://doi.org/10.5194/acp-24-7063-2024, 2024
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The anthropogenic fraction of non-methane volatile organic compound (NMVOC) emissions associated with biogenic sources (e.g., terpenes) is investigated based on eddy covariance observations. The anthropogenic fraction of terpene emissions is strongly dependent on season. When analyzing volatile chemical product (VCP) emissions in urban environments, we caution that observations from short-term campaigns might over-/underestimate their significance depending on local and seasonal circumstances.
Sihang Wang, Bin Yuan, Xianjun He, Ru Cui, Xin Song, Yubin Chen, Caihong Wu, Chaomin Wang, Yibo Huangfu, Xiao-Bing Li, Boguang Wang, and Min Shao
Atmos. Chem. Phys., 24, 7101–7121, https://doi.org/10.5194/acp-24-7101-2024, https://doi.org/10.5194/acp-24-7101-2024, 2024
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Emissions of reactive organic gases from industrial volatile chemical product sources are measured. There are large differences among these industrial sources. We show that oxygenated species account for significant contributions to reactive organic gas emissions, especially for industrial sources utilizing water-borne chemicals.
Qing Yang, Xiao-Bing Li, Bin Yuan, Xiaoxiao Zhang, Yibo Huangfu, Lei Yang, Xianjun He, Jipeng Qi, and Min Shao
Atmos. Chem. Phys., 24, 6865–6882, https://doi.org/10.5194/acp-24-6865-2024, https://doi.org/10.5194/acp-24-6865-2024, 2024
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Online vertical gradient measurements of formic and isocyanic acids were made based on a 320 m tower in a megacity. Vertical variations and sources of the two acids were analyzed in this study. We find that formic and isocyanic acids exhibited positive vertical gradients and were mainly contributed by photochemical formations. The formation of formic and isocyanic acids was also significantly enhanced in urban regions aloft.
Junwei Song, Harald Saathoff, Feng Jiang, Linyu Gao, Hengheng Zhang, and Thomas Leisner
Atmos. Chem. Phys., 24, 6699–6717, https://doi.org/10.5194/acp-24-6699-2024, https://doi.org/10.5194/acp-24-6699-2024, 2024
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This study presents concurrent online measurements of organic gas and particles (VOCs and OA) at a forested site in summer. Both VOCs and OA were largely contributed by oxygenated organic compounds. Semi-volatile oxygenated OA and organic nitrate formed from monoterpenes and sesquiterpenes contributed significantly to nighttime particle growth. The results help us to understand the causes of nighttime particle growth regularly observed in summer in central European rural forested environments.
Xin Yang, Kimberly Strong, Alison S. Criscitiello, Marta Santos-Garcia, Kristof Bognar, Xiaoyi Zhao, Pierre Fogal, Kaley A. Walker, Sara M. Morris, and Peter Effertz
Atmos. Chem. Phys., 24, 5863–5886, https://doi.org/10.5194/acp-24-5863-2024, https://doi.org/10.5194/acp-24-5863-2024, 2024
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This study uses snow samples collected from a Canadian high Arctic site, Eureka, to demonstrate that surface snow in early spring is a net sink of atmospheric bromine and nitrogen. Surface snow bromide and nitrate are significantly correlated, indicating the oxidation of reactive nitrogen is accelerated by reactive bromine. In addition, we show evidence that snow photochemical release of reactive bromine is very weak, and its emission flux is much smaller than the deposition flux of bromide.
Cited articles
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Formaldehyde (HCHO) and Hydroperoxide distribution around the Arabian Peninsula – A comparison of ship-based measurements with the general circulation model EMAC, Atmos. Chem. Phys., in preparation, 2021.
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DiGangi, J. P., Henry, S. B., Kammrath, A., Boyle, E. S., Kaser, L., Schnitzhofer, R., Graus, M., Turnipseed, A., Park, J.-H., Weber, R. J., Hornbrook, R. S., Cantrell, C. A., Maudlin III, R. L., Kim, S., Nakashima, Y., Wolfe, G. M., Kajii, Y., Apel, E. C., Goldstein, A. H., Guenther, A., Karl, T., Hansel, A., and Keutsch, F. N.: Observations of glyoxal and formaldehyde as metrics for the anthropogenic impact on rural photochemistry, Atmos. Chem. Phys., 12, 9529–9543, https://doi.org/10.5194/acp-12-9529-2012, 2012.
Duncan, B. N., Yoshida, Y., Olson, J. R., Sillman, S., Martin, R. V., Lamsal, L., Hu, Y., Pickering, K. E., Retscher, C., Allen, D. J., and Crawford, J. H.:
Application of OMI observations to a space-based indicator of NOx and VOC controls on surface ozone formation,
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Edtbauer, A., Stönner, C., Pfannerstill, E. Y., Berasategui, M., Walter, D., Crowley, J. N., Lelieveld, J., and Williams, J.: A new marine biogenic emission: methane sulfonamide (MSAM), dimethyl sulfide (DMS), and dimethyl sulfone (DMSO2) measured in air over the Arabian Sea, Atmos. Chem. Phys., 20, 6081–6094, https://doi.org/10.5194/acp-20-6081-2020, 2020.
Eger, P. G., Friedrich, N., Schuladen, J., Shenolikar, J., Fischer, H., Tadic, I., Harder, H., Martinez, M., Rohloff, R., Tauer, S., Drewnick, F., Fachinger, F., Brooks, J., Darbyshire, E., Sciare, J., Pikridas, M., Lelieveld, J., and Crowley, J. N.: Shipborne measurements of ClNO2 in the Mediterranean Sea and around the Arabian Peninsula during summer, Atmos. Chem. Phys., 19, 12121–12140, https://doi.org/10.5194/acp-19-12121-2019, 2019.
Fortems-Cheiney, A., Chevallier, F., Pison, I., Bousquet, P., Saunois, M., Szopa, S., Cressot, C., Kurosu, T. P., Chance, K., and Fried, A.: The formaldehyde budget as seen by a global-scale multi-constraint and multi-species inversion system, Atmos. Chem. Phys., 12, 6699–6721, https://doi.org/10.5194/acp-12-6699-2012, 2012.
Fried, A., Cantrell, C., Olson, J., Crawford, J. H., Weibring, P., Walega, J., Richter, D., Junkermann, W., Volkamer, R., Sinreich, R., Heikes, B. G., O'Sullivan, D., Blake, D. R., Blake, N., Meinardi, S., Apel, E., Weinheimer, A., Knapp, D., Perring, A., Cohen, R. C., Fuelberg, H., Shetter, R. E., Hall, S. R., Ullmann, K., Brune, W. H., Mao, J., Ren, X., Huey, L. G., Singh, H. B., Hair, J. W., Riemer, D., Diskin, G., and Sachse, G.: Detailed comparisons of airborne formaldehyde measurements with box models during the 2006 INTEX-B and MILAGRO campaigns: potential evidence for significant impacts of unmeasured and multi-generation volatile organic carbon compounds, Atmos. Chem. Phys., 11, 11867–11894, https://doi.org/10.5194/acp-11-11867-2011, 2011.
Friedrich, N., Eger, P., Shenolikar, J., Sobanski, N., Schuladen, J., Dienhart, D., Hottmann, B., Tadic, I., Fischer, H., Martinez, M., Rohloff, R., Tauer, S., Harder, H., Pfannerstill, E. Y., Wang, N., Williams, J., Brooks, J., Drewnick, F., Su, H., Li, G., Cheng, Y., Lelieveld, J., and Crowley, J. N.: Reactive nitrogen around the Arabian Peninsula and in the Mediterranean Sea during the 2017 AQABA ship campaign, Atmos. Chem. Phys., 21, 7473–7498, https://doi.org/10.5194/acp-21-7473-2021, 2021.
Fuchs, H., Novelli, A., Rolletter, M., Hofzumahaus, A., Pfannerstill, E. Y., Kessel, S., Edtbauer, A., Williams, J., Michoud, V., Dusanter, S., Locoge, N., Zannoni, N., Gros, V., Truong, F., Sarda-Esteve, R., Cryer, D. R., Brumby, C. A., Whalley, L. K., Stone, D., Seakins, P. W., Heard, D. E., Schoemaecker, C., Blocquet, M., Coudert, S., Batut, S., Fittschen, C., Thames, A. B., Brune, W. H., Ernest, C., Harder, H., Muller, J. B. A., Elste, T., Kubistin, D., Andres, S., Bohn, B., Hohaus, T., Holland, F., Li, X., Rohrer, F., Kiendler-Scharr, A., Tillmann, R., Wegener, R., Yu, Z., Zou, Q., and Wahner, A.: Comparison of OH reactivity measurements in the atmospheric simulation chamber SAPHIR, Atmos. Meas. Tech., 10, 4023–4053, https://doi.org/10.5194/amt-10-4023-2017, 2017.
Hens, K., Novelli, A., Martinez, M., Auld, J., Axinte, R., Bohn, B., Fischer, H., Keronen, P., Kubistin, D., Nölscher, A. C., Oswald, R., Paasonen, P., Petäjä, T., Regelin, E., Sander, R., Sinha, V., Sipilä, M., Taraborrelli, D., Tatum Ernest, C., Williams, J., Lelieveld, J., and Harder, H.: Observation and modelling of HOx radicals in a boreal forest, Atmos. Chem. Phys., 14, 8723–8747, https://doi.org/10.5194/acp-14-8723-2014, 2014.
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Kormann, R., Fischer, H., de Reus, M., Lawrence, M., Brühl, Ch., von Kuhlmann, R., Holzinger, R., Williams, J., Lelieveld, J., Warneke, C., de Gouw, J., Heland, J., Ziereis, H., and Schlager, H.: Formaldehyde over the eastern Mediterranean during MINOS: Comparison of airborne in-situ measurements with 3D-model results, Atmos. Chem. Phys., 3, 851–861, https://doi.org/10.5194/acp-3-851-2003, 2003.
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Marno, D., Ernest, C., Hens, K., Javed, U., Klimach, T., Martinez, M., Rudolf, M., Lelieveld, J., and Harder, H.: Calibration of an airborne HOx instrument using the All Pressure Altitude-based Calibrator for HOx Experimentation (APACHE), Atmos. Meas. Tech., 13, 2711–2731, https://doi.org/10.5194/amt-13-2711-2020, 2020.
Martin, R. V., Fiore, A. M., and Van Donkelaar, A.:
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Palmer, P. I., Jacob, D. J., Fiore, A. M., Martin, R. V., Chance, K., and Kurosu, T. P.:
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Pfannerstill, E. Y., Wang, N., and Williams, J.: Total OH reactivity measured around the Arabian Peninsula July-August 2017, 3.2, Zenodo [data set], https://doi.org/10.5281/zenodo.3354117, 2019.
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Tadic, I., Crowley, J. N., Dienhart, D., Eger, P., Harder, H., Hottmann, B., Martinez, M., Parchatka, U., Paris, J.-D., Pozzer, A., Rohloff, R., Schuladen, J., Shenolikar, J., Tauer, S., Lelieveld, J., and Fischer, H.: Net ozone production and its relationship to nitrogen oxides and volatile organic compounds in the marine boundary layer around the Arabian Peninsula, Atmos. Chem. Phys., 20, 6769–6787, https://doi.org/10.5194/acp-20-6769-2020, 2020.
Tegtmeier, S., Marandino, C., Jia, Y., Quack, B., and Mahajan, A. S.: Atmospheric gas-phase composition over the Indian Ocean, Atmos. Chem. Phys. Discuss. [preprint], https://doi.org/10.5194/acp-2020-718, in review, 2020.
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Are CH2O measurements in the marine boundary layer suitable for testing the current understanding of CH4 photooxidation?: A model study,
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Short summary
We present the first ship-based in situ measurements of formaldehyde (HCHO), hydroxyl radicals (OH) and the OH reactivity around the Arabian Peninsula. Regression analysis of the HCHO production rate and the related OH chemistry revealed the regional HCHO yield αeff, which represents the different chemical regimes encountered. Highest values were found for the Arabian Gulf (also known as the Persian Gulf), which highlights this region as a hotspot of photochemical air pollution.
We present the first ship-based in situ measurements of formaldehyde (HCHO), hydroxyl radicals...
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