Articles | Volume 15, issue 12
https://doi.org/10.5194/acp-15-6971-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-15-6971-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
29 Jun 2015
Research article |
| 29 Jun 2015
Hydrogen peroxide in the marine boundary layer over the South Atlantic during the OOMPH cruise in March 2007
H. Fischer
CORRESPONDING AUTHOR
Max Planck Institute for Chemistry, Department of Atmospheric Chemistry, Mainz, Germany
A. Pozzer
Max Planck Institute for Chemistry, Department of Atmospheric Chemistry, Mainz, Germany
T. Schmitt
Max Planck Institute for Chemistry, Department of Atmospheric Chemistry, Mainz, Germany
P. Jöckel
Deutsches Zentrum für Luft- und Raumfahrt (DLR), Institut für Physik der Atmosphäre, Oberpfaffenhofen, Germany
T. Klippel
Max Planck Institute for Chemistry, Department of Atmospheric Chemistry, Mainz, Germany
D. Taraborrelli
Max Planck Institute for Chemistry, Department of Atmospheric Chemistry, Mainz, Germany
J. Lelieveld
Max Planck Institute for Chemistry, Department of Atmospheric Chemistry, Mainz, Germany
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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
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Nils Friedrich, Ivan Tadic, Jan Schuladen, James Brooks, Eoghan Darbyshire, Frank Drewnick, Horst Fischer, Jos Lelieveld, and John N. Crowley
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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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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.
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.
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.
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.
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.
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.
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.
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.
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.
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.
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.
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
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.
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.
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.
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.
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.
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
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
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
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
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
Simon Rosanka, Holger Tost, Rolf Sander, Patrick Jöckel, Astrid Kerkweg, and Domenico Taraborrelli
Geosci. Model Dev., 17, 2597–2615, https://doi.org/10.5194/gmd-17-2597-2024, https://doi.org/10.5194/gmd-17-2597-2024, 2024
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The capabilities of the Modular Earth Submodel System (MESSy) are extended to account for non-equilibrium aqueous-phase chemistry in the representation of deliquescent aerosols. When applying the new development in a global simulation, we find that MESSy's bias in modelling routinely observed reduced inorganic aerosol mass concentrations, especially in the United States. Furthermore, the representation of fine-aerosol pH is particularly improved in the marine boundary layer.
Sergio Soler, Francisco J. Gordillo-Vázquez, Francisco J. Pérez-Invernón, Patrick Jöckel, Torsten Neubert, Olivier Chanrion, Victor Reglero, and Nikolai Østgaard
EGUsphere, https://doi.org/10.5194/egusphere-2024-132, https://doi.org/10.5194/egusphere-2024-132, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Sudden local ozone (O3) enhancements have been reported in different regions of the world since the 1970s. While the hot channel of lightning strokes directly produce significant amounts of nitrogen oxide, no direct emission of O3 is expected. Corona discharges in convectively active regions could explain local O3 increases, which remains unexplained. We present the first mathematical functions that relate the global annual frequency of in-cloud coronas with four sets of meteorological variables
Francisco J. Pérez-Invernón, Francisco J. Gordillo-Vázquez, Alejandro Malagón-Romero, and Patrick Jöckel
Atmos. Chem. Phys., 24, 3577–3592, https://doi.org/10.5194/acp-24-3577-2024, https://doi.org/10.5194/acp-24-3577-2024, 2024
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Sprites are electrical discharges that occur in the upper atmosphere. Recent modelling and observational data suggest that they may have a measurable impact on atmospheric chemistry. We incorporate both the occurrence rate of sprites and their production of chemical species into a chemistry–climate model. While our results indicate that sprites have a minimal global influence on atmospheric chemistry, they underscore their noteworthy importance at a regional scale.
Yasin Elshorbany, Jerald Ziemke, Sarah Strode, Hervé Petetin, Kazuyuki Miyazaki, Isabelle De Smedt, Kenneth Pickering, Rodrigo Seguel, Helen Worden, Tamara Emmerichs, Domenico Taraborrelli, Maria Cazorla, Suvarna Fadnavis, Rebecca Buchholz, Benjamin Gaubert, Néstor Rojas, Thiago Nogueira, Thérèse Salameh, and Min Huang
EGUsphere, https://doi.org/10.5194/egusphere-2024-720, https://doi.org/10.5194/egusphere-2024-720, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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We investigated tropospheric ozone spatial variability and trends from 2005 to 2019 and related those to ozone precursors on global and regional scales. We also investigate the spatiotemporal characteristics of the ozone formation regime in relation to ozone chemical sources and sinks. Our analysis is based on remote sensing products of the Tropospheric Column of Ozone and its precursors, nitrogen dioxide, formaldehyde, and total column of CO as well as ozonesonde data and model simulations.
Xiaodan Ma, Jianping Huang, Michaela Hegglin, Patrick Joeckel, and Tianliang Zhao
EGUsphere, https://doi.org/10.5194/egusphere-2023-2411, https://doi.org/10.5194/egusphere-2023-2411, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Our study examines 30 years of tropospheric ozone changes in the Northwest Pacific region. We found a significant increase in ozone levels during spring and summer in the middle-upper troposphere. This change is driven by a complex interplay between stratospheric and tropospheric ozone, with implications for climate and air quality in East Asia. Further research into these mechanisms is needed.
Georgia Lazoglou, Theo Economou, Christina Anagnostopoulou, George Zittis, Anna Tzyrkalli, Pantelis Georgiades, and Jos Lelieveld
EGUsphere, https://doi.org/10.5194/egusphere-2024-45, https://doi.org/10.5194/egusphere-2024-45, 2024
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This study focused on the important issue of the drizzle bias effect in regional climate models, described by an over-prediction of the number of rainy days while underestimating associated precipitation amounts. For this purpose, two distinct methodologies were applied and rigorously evaluated. These results are encouraging for using the multivariate machine learning method of Random Forest for increasing the accuracy of climate models, concerning the projection of the number of wet days.
Simone Rodrigues, Glauber Cirino, Demerval Moreira, Andrea Pozzer, Rafael Palácios, Sung-Ching Lee, Breno Imbiriba, José Nogueira, Maria Isabel Vitorino, and George Vourlitis
Biogeosciences, 21, 843–868, https://doi.org/10.5194/bg-21-843-2024, https://doi.org/10.5194/bg-21-843-2024, 2024
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The radiative effects of atmospheric particles are still unknown for a wide variety of species and types of vegetation present in Amazonian biomes. We examined the effects of aerosols on solar radiation and their impacts on photosynthesis in an area of semideciduous forest in the southern Amazon Basin. Under highly smoky-sky conditions, our results show substantial photosynthetic interruption (20–70 %), attributed specifically to the decrease in solar radiation and leaf canopy temperature.
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.
Mariano Mertens, Sabine Brinkop, Phoebe Graf, Volker Grewe, Johannes Hendricks, Patrick Jöckel, Anna Lanteri, Sigrun Matthes, Vanessa S. Rieger, Mattia Righi, and Robin N. Thor
EGUsphere, https://doi.org/10.5194/egusphere-2024-324, https://doi.org/10.5194/egusphere-2024-324, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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We quantified the contributions of land transport, shipping and aviation emissions to tropospheric ozone and the reductions of the methane lifetime using chemistry-climate model simulations. The contributions were analysed for the conditions of 2015 and for three projections for the year 2050. The results highllight the challenges of mitigating ozone formed by emissions of the transport sector, caused by the non-linearitiy of the ozone chemistry and the long life-time.
Ryan S. Williams, Michaela I. Hegglin, Patrick Jöckel, Hella Garny, and Keith P. Shine
Atmos. Chem. Phys., 24, 1389–1413, https://doi.org/10.5194/acp-24-1389-2024, https://doi.org/10.5194/acp-24-1389-2024, 2024
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During winter, a brief but abrupt reversal of the mean stratospheric westerly flow (~30 km high) around the Arctic occurs ~6 times a decade. Using a chemistry–climate model, about half of these events are shown to induce large anomalies in Arctic ozone (>25 %) and water vapour (>±25 %) around ~8–12 km altitude for up to 2–3 months, important for weather forecasting. We also calculate a doubling to trebling of the risk in breaches of mid-latitude surface air quality (ozone) standards (~60 ppbv).
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
EGUsphere, https://doi.org/10.5194/egusphere-2023-2848, https://doi.org/10.5194/egusphere-2023-2848, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Through measurements of various trace gases in a sub-urban 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/physical loss processes. NO was observed as a result of nighttime soil emissions when ozone 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 nitrogen.
Luiz A. T. Machado, Jürgen Kesselmeier, Santiago Botia, Hella Van Asperen, Alessandro C. de Araújo, Paulo Artaxo, Achim Edtbauer, Rosa Ferreira, Hartwig Harder, Sam Jones, Cléo Q. Dias-Júnior, Guido G. Haytzmann, Carlos A. Quesada, Shujiro Komiya, Jost Lavric, Jos Lelieveld, Ingeborg Levin, Anke Nölscher, Eva Pfannerstill, Mira Pöhlker, Ulrich Pöschl, Akima Ringsdorf, Luciana Rizzo, Ana M. Yáñez-Serrano, Susan Trumbore, Wanda I. D. Valenti, Jordi Vila-Guerau de Arellano, David Walter, Jonathan Williams, Stefan Wolff, and Christopher Pöhlker
EGUsphere, https://doi.org/10.5194/egusphere-2023-2901, https://doi.org/10.5194/egusphere-2023-2901, 2024
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Composite analysis of the gas concentration before and after rainfall, during the day and night, gives insight into the complex relationship between trace gas variability and precipitation. This analysis helps to understand the sources and sinks of trace gases within a forest ecosystem. It elucidates processes that are not discernible under undisturbed conditions and contributes to a deeper understanding of the trace gas life cycle and its intricate interactions with cloud dynamics in the Amazon
Philipp Joppe, Johannes Schneider, Katharina Kaiser, Horst Fischer, Peter Hoor, Daniel Kunkel, Hans-Christoph Lachnitt, Andreas Marsing, Lenard Röder, Hans Schlager, Laura Tomsche, Christiane Voigt, Andreas Zahn, and Stephan Borrmann
EGUsphere, https://doi.org/10.5194/egusphere-2024-7, https://doi.org/10.5194/egusphere-2024-7, 2024
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From aircraft measurements in the upper troposphere/lower stratosphere we find a correlation between the ozone and particulate sulfate in the lower stratosphere. The correlation exhibits some variability over the measurement period exceeding the background sulfate to ozone correlation. From our analysis, we conclude that gas-to-particle conversion of volcanic sulfur dioxide leads to the observed enhanced sulfate aerosol mixing ratios.
Leon Kuhn, Steffen Beirle, Vinod Kumar, Sergey Osipov, Andrea Pozzer, Tim Bösch, Rajesh Kumar, and Thomas Wagner
Atmos. Chem. Phys., 24, 185–217, https://doi.org/10.5194/acp-24-185-2024, https://doi.org/10.5194/acp-24-185-2024, 2024
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NO₂ is an important air pollutant. It was observed that the WRF-Chem model shows significant deviations in NO₂ abundance when compared to measurements. We use a 1-month simulation over central Europe to show that these deviations can be mostly resolved by reparameterization of the vertical mixing routine. In order to validate our results, they are compared to in situ, satellite, and MAX-DOAS measurements.
Anna Martin, Veronika Gayler, Benedikt Steil, Klaus Klingmüller, Patrick Jöckel, Holger Tost, Jos Lelieveld, and Andrea Pozzer
EGUsphere, https://doi.org/10.5194/egusphere-2023-3051, https://doi.org/10.5194/egusphere-2023-3051, 2024
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The study evaluates the land surface and vegetation model JSBACHv4 as a replacement for the simplified submodel SURFACE in EMAC. JSBACH mitigates earlier problems of soil dryness, which are critical for vegetation modelling. When analysed with different data sets, the coupled model shows strong correlations for key variables such as land surface temperature, surface albedo and radiation flux. The versatility of the model is significantly increased, while the overall performance is not degraded.
Meghna Soni, Rolf Sander, Lokesh K. Sahu, Domenico Taraborrelli, Pengfei Liu, Ankit Patel, Imran A. Girach, Andrea Pozzer, Sachin S. Gunthe, and Narendra Ojha
Atmos. Chem. Phys., 23, 15165–15180, https://doi.org/10.5194/acp-23-15165-2023, https://doi.org/10.5194/acp-23-15165-2023, 2023
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The study presents the implementation of comprehensive multiphase chlorine chemistry in the box model CAABA/MECCA. Simulations for contrasting urban environments of Asia and Europe highlight the significant impacts of chlorine on atmospheric oxidation capacity and composition. Chemical processes governing the production and loss of chlorine-containing species has been discussed. The updated chemical mechanism will be useful to interpret field measurements and for future air quality studies.
Linda Ort, Lenard Lukas Röder, Uwe Parchatka, Rainer Königstedt, Daniel Crowley, Frank Kunz, Ralf Wittkowski, Jos Lelieveld, and Horst Fischer
EGUsphere, https://doi.org/10.5194/egusphere-2023-2842, https://doi.org/10.5194/egusphere-2023-2842, 2023
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Airborne in-situ measurements are of great importance to collect valuable atmospheric data to improve our knowledge of existing processes, but also hold challenges which demand specific designs. This study presents an IR spectrometer for airborne trace gas measurements with high data efficiency and a simple, compact design. Its performance is characterized with the help of a test flight and a comparison with another spectrometer. Moreover, results from its first campaign highlight its benefits.
Matthias Nützel, Laura Stecher, Patrick Jöckel, Franziska Winterstein, Martin Dameris, Michael Ponater, Phoebe Graf, and Markus Kunze
EGUsphere, https://doi.org/10.5194/egusphere-2023-2140, https://doi.org/10.5194/egusphere-2023-2140, 2023
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We extended the infrastructure of our modelling system to enable the use of an additional radiation scheme. After calibrating the model setups to the old and the new radiation scheme, we find that the simulation with the new scheme shows considerable improvements e.g. concerning the cold point temperature and stratospheric water vapour. Further, perturbations of radiative fluxes associated with greenhouse gas changes, e.g. of methane, tend to be improved when the new scheme is employed.
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°.
Tamara Emmerichs, Yen-Sen Lu, and Domenico Taraborrelli
EGUsphere, https://doi.org/10.5194/egusphere-2023-2306, https://doi.org/10.5194/egusphere-2023-2306, 2023
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We assess the representation of the plant' response to surface water in a global atmospheric chemistry model. This sensitivity is crucial for the return of precipitation back to the atmosphere and thus significantly impacts the representation of weather as well as air quality. The newly implemented response function reduces this process towards a better comparison with satellite observations. This yields a higher intensity of unusual warm periods and a higher production of air pollutants.
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.
Roland Eichinger, Sebastian Rhode, Hella Garny, Peter Preusse, Petr Pisoft, Aleš Kuchař, Patrick Jöckel, Astrid Kerkweg, and Bastian Kern
Geosci. Model Dev., 16, 5561–5583, https://doi.org/10.5194/gmd-16-5561-2023, https://doi.org/10.5194/gmd-16-5561-2023, 2023
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The columnar approach of gravity wave (GW) schemes results in dynamical model biases, but parallel decomposition makes horizontal GW propagation computationally unfeasible. In the global model EMAC, we approximate it by GW redistribution at one altitude using tailor-made redistribution maps generated with a ray tracer. More spread-out GW drag helps reconcile the model with observations and close the 60°S GW gap. Polar vortex dynamics are improved, enhancing climate model credibility.
Marc von Hobe, Domenico Taraborrelli, Sascha Alber, Birger Bohn, Hans-Peter Dorn, Hendrik Fuchs, Yun Li, Chenxi Qiu, Franz Rohrer, Roberto Sommariva, Fred Stroh, Zhaofeng Tan, Sergej Wedel, and Anna Novelli
Atmos. Chem. Phys., 23, 10609–10623, https://doi.org/10.5194/acp-23-10609-2023, https://doi.org/10.5194/acp-23-10609-2023, 2023
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The trace gas carbonyl sulfide (OCS) transports sulfur from the troposphere to the stratosphere, where sulfate aerosols are formed that influence climate and stratospheric chemistry. An uncertain OCS source in the troposphere is chemical production form dimethyl sulfide (DMS), a gas released in large quantities from the oceans. We carried out experiments in a large atmospheric simulation chamber to further elucidate the chemical mechanism of OCS production from DMS.
Marina Friedel, Gabriel Chiodo, Timofei Sukhodolov, James Keeble, Thomas Peter, Svenja Seeber, Andrea Stenke, Hideharu Akiyoshi, Eugene Rozanov, David Plummer, Patrick Jöckel, Guang Zeng, Olaf Morgenstern, and Béatrice Josse
Atmos. Chem. Phys., 23, 10235–10254, https://doi.org/10.5194/acp-23-10235-2023, https://doi.org/10.5194/acp-23-10235-2023, 2023
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Previously, it has been suggested that springtime Arctic ozone depletion might worsen in the coming decades due to climate change, which might counteract the effect of reduced ozone-depleting substances. Here, we show with different chemistry–climate models that springtime Arctic ozone depletion will likely decrease in the future. Further, we explain why models show a large spread in the projected development of Arctic ozone depletion and use the model spread to constrain future projections.
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.
Markus Kilian, Volker Grewe, Patrick Jöckel, Astrid Kerkweg, Mariano Mertens, Andreas Zahn, and Helmut Ziereis
EGUsphere, https://doi.org/10.5194/egusphere-2023-528, https://doi.org/10.5194/egusphere-2023-528, 2023
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Anthropogenic emissions are a major source of precursors for tropospheric ozone formation. As ozone formation is highly non-linear, we apply a global-regional chemistry-climate model with a source attribution method (tagging) to quantify the contribution of anthropogenic emissions to ozone. We focus on two major polluted areas in Europe, the Po Valley and the Benelux region. Our analysis shows that in particular anthropogenic emissions from Europe contribute largely to ground-level ozone.
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.
Felix Wieser, Rolf Sander, and Domenico Taraborrelli
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2023-102, https://doi.org/10.5194/gmd-2023-102, 2023
Revised manuscript accepted for GMD
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The chemistry scheme of the atmospheric box model CAABA/MECCA was expanded to achieve an improved aerosol formation from emitted organic compounds. In addition to newly added reactions, temperature-dependent partitioning of all new species between the gas and aqueous phase was estimated and included in the preexisting scheme. Sensitivity runs show an overestimation of key compounds from isoprene, which can be explained by a lack of aqueous phase degradation reactions and box model limitations.
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.
Robin N. Thor, Mariano Mertens, Sigrun Matthes, Mattia Righi, Johannes Hendricks, Sabine Brinkop, Phoebe Graf, Volker Grewe, Patrick Jöckel, and Steven Smith
Geosci. Model Dev., 16, 1459–1466, https://doi.org/10.5194/gmd-16-1459-2023, https://doi.org/10.5194/gmd-16-1459-2023, 2023
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We report on an inconsistency in the latitudinal distribution of aviation emissions between two versions of a data product which is widely used by researchers. From the available documentation, we do not expect such an inconsistency. We run a chemistry–climate model to compute the effect of the inconsistency in emissions on atmospheric chemistry and radiation and find that the radiative forcing associated with aviation ozone is 7.6 % higher when using the less recent version of the data.
Dominik Brunner, Gerrit Kuhlmann, Stephan Henne, Erik Koene, Bastian Kern, Sebastian Wolff, Christiane Voigt, Patrick Jöckel, Christoph Kiemle, Anke Roiger, Alina Fiehn, Sven Krautwurst, Konstantin Gerilowski, Heinrich Bovensmann, Jakob Borchardt, Michal Galkowski, Christoph Gerbig, Julia Marshall, Andrzej Klonecki, Pascal Prunet, Robert Hanfland, Margit Pattantyús-Ábrahám, Andrzej Wyszogrodzki, and Andreas Fix
Atmos. Chem. Phys., 23, 2699–2728, https://doi.org/10.5194/acp-23-2699-2023, https://doi.org/10.5194/acp-23-2699-2023, 2023
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We evaluated six atmospheric transport models for their capability to simulate the CO2 plumes from two of the largest power plants in Europe by comparing the models against aircraft observations collected during the CoMet (Carbon Dioxide and Methane Mission) campaign in 2018. The study analyzed how realistically such plumes can be simulated at different model resolutions and how well the planned European satellite mission CO2M will be able to quantify emissions from power plants.
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.
Flora Kluge, Tilman Hüneke, Christophe Lerot, Simon Rosanka, Meike K. Rotermund, Domenico Taraborrelli, Benjamin Weyland, and Klaus Pfeilsticker
Atmos. Chem. Phys., 23, 1369–1401, https://doi.org/10.5194/acp-23-1369-2023, https://doi.org/10.5194/acp-23-1369-2023, 2023
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Using airborne glyoxal concentration and vertical column density measurements, vertical profiles are inferred for eight global regions in aged biomass burning plumes and the tropical marine boundary layer. Using TROPOMI observations, an analysis of space- and airborne measurements is performed. A comparison to EMAC simulations shows a general glyoxal underprediction, which points to various missing sources and precursors from anthropogenic activities, biomass burning, and the sea surface.
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.
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.
Manuel Schlund, Birgit Hassler, Axel Lauer, Bouwe Andela, Patrick Jöckel, Rémi Kazeroni, Saskia Loosveldt Tomas, Brian Medeiros, Valeriu Predoi, Stéphane Sénési, Jérôme Servonnat, Tobias Stacke, Javier Vegas-Regidor, Klaus Zimmermann, and Veronika Eyring
Geosci. Model Dev., 16, 315–333, https://doi.org/10.5194/gmd-16-315-2023, https://doi.org/10.5194/gmd-16-315-2023, 2023
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The Earth System Model Evaluation Tool (ESMValTool) is a community diagnostics and performance metrics tool for routine evaluation of Earth system models. Originally, ESMValTool was designed to process reformatted output provided by large model intercomparison projects like the Coupled Model Intercomparison Project (CMIP). Here, we describe a new extension of ESMValTool that allows for reading and processing native climate model output, i.e., data that have not been reformatted before.
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.
Matthias Nützel, Sabine Brinkop, Martin Dameris, Hella Garny, Patrick Jöckel, Laura L. Pan, and Mijeong Park
Atmos. Chem. Phys., 22, 15659–15683, https://doi.org/10.5194/acp-22-15659-2022, https://doi.org/10.5194/acp-22-15659-2022, 2022
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During the Asian summer monsoon season, a large high-pressure system is present at levels close to the tropopause above Asia. We analyse how air masses are transported from surface levels to this high-pressure system, which shows distinct features from the surrounding air masses. To this end, we employ multiannual data from two complementary models that allow us to analyse the climatology as well as the interannual and intraseasonal variability of these transport pathways.
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.
Johannes Pletzer, Didier Hauglustaine, Yann Cohen, Patrick Jöckel, and Volker Grewe
Atmos. Chem. Phys., 22, 14323–14354, https://doi.org/10.5194/acp-22-14323-2022, https://doi.org/10.5194/acp-22-14323-2022, 2022
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Very fast aircraft can travel long distances in extremely short times and can fly at high altitudes (15 to 35 km). These aircraft emit water vapour, nitrogen oxides, and hydrogen. Water vapour emissions remain for months to several years at these altitudes and have an important impact on temperature. We investigate two aircraft fleets flying at 26 and 35 km. Ozone is depleted more, and the water vapour perturbation and temperature change are larger for the aircraft flying at 35 km.
Jin Maruhashi, Volker Grewe, Christine Frömming, Patrick Jöckel, and Irene C. Dedoussi
Atmos. Chem. Phys., 22, 14253–14282, https://doi.org/10.5194/acp-22-14253-2022, https://doi.org/10.5194/acp-22-14253-2022, 2022
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Aviation NOx emissions lead to the formation of ozone in the atmosphere in the short term, which has a climate warming effect. This study uses global-scale simulations to characterize the transport patterns between NOx emissions at an altitude of ~ 10.4 km and the resulting ozone. Results show a strong spatial and temporal dependence of NOx in disturbing atmospheric O3 concentrations, with the location that is most impacted in terms of warming not necessarily coinciding with the emission region.
Kostas Eleftheratos, John Kapsomenakis, Ilias Fountoulakis, Christos S. Zerefos, Patrick Jöckel, Martin Dameris, Alkiviadis F. Bais, Germar Bernhard, Dimitra Kouklaki, Kleareti Tourpali, Scott Stierle, J. Ben Liley, Colette Brogniez, Frédérique Auriol, Henri Diémoz, Stana Simic, Irina Petropavlovskikh, Kaisa Lakkala, and Kostas Douvis
Atmos. Chem. Phys., 22, 12827–12855, https://doi.org/10.5194/acp-22-12827-2022, https://doi.org/10.5194/acp-22-12827-2022, 2022
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We present the future evolution of DNA-active ultraviolet (UV) radiation in view of increasing greenhouse gases (GHGs) and decreasing ozone depleting substances (ODSs). It is shown that DNA-active UV radiation might increase after 2050 between 50° N–50° S due to GHG-induced reductions in clouds and ozone, something that is likely not to happen at high latitudes, where DNA-active UV radiation will continue its downward trend mainly due to stratospheric ozone recovery from the reduction in ODSs.
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.
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.
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 %.
Francisco J. Pérez-Invernón, Heidi Huntrieser, Thilo Erbertseder, Diego Loyola, Pieter Valks, Song Liu, Dale J. Allen, Kenneth E. Pickering, Eric J. Bucsela, Patrick Jöckel, Jos van Geffen, Henk Eskes, Sergio Soler, Francisco J. Gordillo-Vázquez, and Jeff Lapierre
Atmos. Meas. Tech., 15, 3329–3351, https://doi.org/10.5194/amt-15-3329-2022, https://doi.org/10.5194/amt-15-3329-2022, 2022
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Lightning, one of the major sources of nitrogen oxides in the atmosphere, contributes to the tropospheric concentration of ozone and to the oxidizing capacity of the atmosphere. In this work, we contribute to improving the estimation of lightning-produced nitrogen oxides in the Ebro Valley and the Pyrenees by using two different TROPOMI products and comparing the results.
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.
Dimitris Akritidis, Andrea Pozzer, Johannes Flemming, Antje Inness, Philippe Nédélec, and Prodromos Zanis
Atmos. Chem. Phys., 22, 6275–6289, https://doi.org/10.5194/acp-22-6275-2022, https://doi.org/10.5194/acp-22-6275-2022, 2022
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We perform a process-oriented evaluation of Copernicus Atmosphere Monitoring Service (CAMS) reanalysis (CAMSRA) O3 over Europe using WOUDC (World Ozone and Ultraviolet Radiation Data Centre) ozonesondes and IAGOS (In-service Aircraft for a Global Observing System) aircraft measurements. Chemical data assimilation assists CAMSRA to reproduce the observed O3 increases in the troposphere during the examined folding events, but it mostly results in O3 overestimation in the upper troposphere.
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.
M. Dolores Andrés Hernández, Andreas Hilboll, Helmut Ziereis, Eric Förster, Ovid O. Krüger, Katharina Kaiser, Johannes Schneider, Francesca Barnaba, Mihalis Vrekoussis, Jörg Schmidt, Heidi Huntrieser, Anne-Marlene Blechschmidt, Midhun George, Vladyslav Nenakhov, Theresa Harlass, Bruna A. Holanda, Jennifer Wolf, Lisa Eirenschmalz, Marc Krebsbach, Mira L. Pöhlker, Anna B. Kalisz Hedegaard, Linlu Mei, Klaus Pfeilsticker, Yangzhuoran Liu, Ralf Koppmann, Hans Schlager, Birger Bohn, Ulrich Schumann, Andreas Richter, Benjamin Schreiner, Daniel Sauer, Robert Baumann, Mariano Mertens, Patrick Jöckel, Markus Kilian, Greta Stratmann, Christopher Pöhlker, Monica Campanelli, Marco Pandolfi, Michael Sicard, José L. Gómez-Amo, Manuel Pujadas, Katja Bigge, Flora Kluge, Anja Schwarz, Nikos Daskalakis, David Walter, Andreas Zahn, Ulrich Pöschl, Harald Bönisch, Stephan Borrmann, Ulrich Platt, and John P. Burrows
Atmos. Chem. Phys., 22, 5877–5924, https://doi.org/10.5194/acp-22-5877-2022, https://doi.org/10.5194/acp-22-5877-2022, 2022
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EMeRGe provides a unique set of in situ and remote sensing airborne measurements of trace gases and aerosol particles along selected flight routes in the lower troposphere over Europe. The interpretation uses also complementary collocated ground-based and satellite measurements. The collected data help to improve the current understanding of the complex spatial distribution of trace gases and aerosol particles resulting from mixing, transport, and transformation of pollution plumes over Europe.
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.
Andrea Pozzer, Simon F. Reifenberg, Vinod Kumar, Bruno Franco, Matthias Kohl, Domenico Taraborrelli, Sergey Gromov, Sebastian Ehrhart, Patrick Jöckel, Rolf Sander, Veronica Fall, Simon Rosanka, Vlassis Karydis, Dimitris Akritidis, Tamara Emmerichs, Monica Crippa, Diego Guizzardi, Johannes W. Kaiser, Lieven Clarisse, Astrid Kiendler-Scharr, Holger Tost, and Alexandra Tsimpidi
Geosci. Model Dev., 15, 2673–2710, https://doi.org/10.5194/gmd-15-2673-2022, https://doi.org/10.5194/gmd-15-2673-2022, 2022
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A newly developed setup of the chemistry general circulation model EMAC (ECHAM5/MESSy for Atmospheric Chemistry) is evaluated here. A comprehensive organic degradation mechanism is used and coupled with a volatility base model.
The results show that the model reproduces most of the tracers and aerosols satisfactorily but shows discrepancies for oxygenated organic gases. It is also shown that this model configuration can be used for further research in atmospheric chemistry.
Francisco J. Pérez-Invernón, Heidi Huntrieser, Patrick Jöckel, and Francisco J. Gordillo-Vázquez
Geosci. Model Dev., 15, 1545–1565, https://doi.org/10.5194/gmd-15-1545-2022, https://doi.org/10.5194/gmd-15-1545-2022, 2022
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This study reports the first parameterization of long-continuing-current lightning in a climate model. Long-continuing-current lightning is proposed to be the main precursor of lightning-ignited wildfires and sprites, a type of transient luminous event taking place in the mesosphere. This parameterization can significantly contribute to improving the implementation of wildfires in climate models.
Guangjie Zheng, Hang Su, Siwen Wang, Andrea Pozzer, and Yafang Cheng
Atmos. Chem. Phys., 22, 47–63, https://doi.org/10.5194/acp-22-47-2022, https://doi.org/10.5194/acp-22-47-2022, 2022
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The recently proposed multiphase buffer theory provides a framework to reconstruct long-term trends and spatial variations in aerosol pH, while non-ideality is a major limitation for its broad applications. Here we proposed a parameterization method to estimate the impact of non-ideality and validated it against long-term observations and global simulations. With this method, the multiphase buffer theory can reproduce well aerosol pH variations estimated by comprehensive thermodynamic models.
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.
Dirk Dienhart, John N. Crowley, Efstratios Bourtsoukidis, Achim Edtbauer, Philipp G. Eger, Lisa Ernle, Hartwig Harder, Bettina Hottmann, Monica Martinez, Uwe Parchatka, Jean-Daniel Paris, Eva Y. Pfannerstill, Roland Rohloff, Jan Schuladen, Christof Stönner, Ivan Tadic, Sebastian Tauer, Nijing Wang, Jonathan Williams, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 17373–17388, https://doi.org/10.5194/acp-21-17373-2021, https://doi.org/10.5194/acp-21-17373-2021, 2021
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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.
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).
Andrea Pozzer
Geosci. Commun., 4, 453–460, https://doi.org/10.5194/gc-4-453-2021, https://doi.org/10.5194/gc-4-453-2021, 2021
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In this paper we investigate the numbers of pages, references and references per page in open-access EGU journals. We showed that, while the number of references and number of pages have been constantly increasing in the period 2010–2020, the number of references per page did not change in the same period. Furthermore, all the journals showed a similar number of references per page, i.e. ~ 3.8 references per page.
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.
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.
Simon Rosanka, Bruno Franco, Lieven Clarisse, Pierre-François Coheur, Andrea Pozzer, Andreas Wahner, and Domenico Taraborrelli
Atmos. Chem. Phys., 21, 11257–11288, https://doi.org/10.5194/acp-21-11257-2021, https://doi.org/10.5194/acp-21-11257-2021, 2021
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The strong El Niño in 2015 led to a particular dry season in Indonesia and favoured severe peatland fires. The smouldering conditions of these fires and the high carbon content of peat resulted in high volatile organic compound (VOC) emissions. By using a comprehensive atmospheric model, we show that these emissions have a significant impact on the tropospheric composition and oxidation capacity. These emissions are transported into to the lower stratosphere, resulting in a depletion of ozone.
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.
Tamara Emmerichs, Bruno Franco, Catherine Wespes, Vinod Kumar, Andrea Pozzer, Simon Rosanka, and Domenico Taraborrelli
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-584, https://doi.org/10.5194/acp-2021-584, 2021
Revised manuscript not accepted
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Near-surface ozone is a harmful air pollutant and it is strongly affected by radical reactions and surface-atmosphere exchanges which in turn are modulated, directly and indirectly, by weather. Understanding the impact of weather on ozone, and air quality, is thus important also in view of weather extremes. The inclusion of additional ozone-weather links in the global model yields a 2-fold reduction of the ozone bias towards satellite observations.
Simon Rosanka, Rolf Sander, Andreas Wahner, and Domenico Taraborrelli
Geosci. Model Dev., 14, 4103–4115, https://doi.org/10.5194/gmd-14-4103-2021, https://doi.org/10.5194/gmd-14-4103-2021, 2021
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The Jülich Aqueous-phase Mechanism of Organic Chemistry (JAMOC) is developed and implemented into the Module Efficiently Calculating the Chemistry of the Atmosphere (MECCA). JAMOC is an explicit in-cloud oxidation scheme for oxygenated volatile organic compounds (OVOCs), which is suitable for global model applications. Within a box-model study, we show that JAMOC yields reduced gas-phase concentrations of most OVOCs and oxidants, except for nitrogen oxides.
Simon Rosanka, Rolf Sander, Bruno Franco, Catherine Wespes, Andreas Wahner, and Domenico Taraborrelli
Atmos. Chem. Phys., 21, 9909–9930, https://doi.org/10.5194/acp-21-9909-2021, https://doi.org/10.5194/acp-21-9909-2021, 2021
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In-cloud destruction of ozone depends on hydroperoxyl radicals in cloud droplets, where they are produced by oxygenated volatile organic compound (OVOC) oxygenation. Only rudimentary representations of these processes, if any, are currently available in global atmospheric models. By using a comprehensive atmospheric model that includes a complex in-cloud OVOC oxidation scheme, we show that atmospheric oxidants are reduced and models ignoring this process will underpredict clouds as ozone sinks.
Christine Frömming, Volker Grewe, Sabine Brinkop, Patrick Jöckel, Amund S. Haslerud, Simon Rosanka, Jesper van Manen, and Sigrun Matthes
Atmos. Chem. Phys., 21, 9151–9172, https://doi.org/10.5194/acp-21-9151-2021, https://doi.org/10.5194/acp-21-9151-2021, 2021
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The influence of weather situations on non-CO2 aviation climate impact is investigated to identify systematic weather-related sensitivities. If aircraft avoid the most sensitive areas, climate impact might be reduced. Enhanced significance is found for emission in relation to high-pressure systems, jet stream, polar night, and tropopause altitude. The results represent a comprehensive data set for studies aiming at weather-dependent flight trajectory optimization to reduce total climate impact.
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.
Jaydeep Singh, Narendra Singh, Narendra Ojha, Amit Sharma, Andrea Pozzer, Nadimpally Kiran Kumar, Kunjukrishnapillai Rajeev, Sachin S. Gunthe, and V. Rao Kotamarthi
Geosci. Model Dev., 14, 1427–1443, https://doi.org/10.5194/gmd-14-1427-2021, https://doi.org/10.5194/gmd-14-1427-2021, 2021
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Atmospheric models often have limitations in simulating the geographically complex and climatically important central Himalayan region. In this direction, we have performed regional modeling at high resolutions to improve the simulation of meteorology and dynamics through a better representation of the topography. The study has implications for further model applications to investigate the effects of anthropogenic pressure over the Himalaya.
Chaim I. Garfinkel, Ohad Harari, Shlomi Ziskin Ziv, Jian Rao, Olaf Morgenstern, Guang Zeng, Simone Tilmes, Douglas Kinnison, Fiona M. O'Connor, Neal Butchart, Makoto Deushi, Patrick Jöckel, Andrea Pozzer, and Sean Davis
Atmos. Chem. Phys., 21, 3725–3740, https://doi.org/10.5194/acp-21-3725-2021, https://doi.org/10.5194/acp-21-3725-2021, 2021
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Water vapor is the dominant greenhouse gas in the atmosphere, and El Niño is the dominant mode of variability in the ocean–atmosphere system. The connection between El Niño and water vapor above ~ 17 km is unclear, with single-model studies reaching a range of conclusions. This study examines this connection in 12 different models. While there are substantial differences among the models, all models appear to capture the fundamental physical processes correctly.
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.
Patrick E. Sheese, Kaley A. Walker, Chris D. Boone, Doug A. Degenstein, Felicia Kolonjari, David Plummer, Douglas E. Kinnison, Patrick Jöckel, and Thomas von Clarmann
Atmos. Meas. Tech., 14, 1425–1438, https://doi.org/10.5194/amt-14-1425-2021, https://doi.org/10.5194/amt-14-1425-2021, 2021
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Output from climate chemistry models (CMAM, EMAC, and WACCM) is used to estimate the expected geophysical variability of ozone concentrations between coincident satellite instrument measurement times and geolocations. We use the Canadian ACE-FTS and OSIRIS instruments as a case study. Ensemble mean estimates are used to optimize coincidence criteria between the two instruments, allowing for the use of more coincident profiles while providing an estimate of the geophysical variation.
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.
Franziska Winterstein and Patrick Jöckel
Geosci. Model Dev., 14, 661–674, https://doi.org/10.5194/gmd-14-661-2021, https://doi.org/10.5194/gmd-14-661-2021, 2021
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Atmospheric methane is currently a hot topic in climate research. This is partly due to its chemically active nature. We introduce a simplified approach to simulate methane in climate models to enable large sensitivity studies by reducing computational cost but including the crucial feedback of methane on stratospheric water vapour. We further provide options to simulate the isotopic content of methane and to generate output for an inverse optimization technique for emission estimation.
Tamara Emmerichs, Astrid Kerkweg, Huug Ouwersloot, Silvano Fares, Ivan Mammarella, and Domenico Taraborrelli
Geosci. Model Dev., 14, 495–519, https://doi.org/10.5194/gmd-14-495-2021, https://doi.org/10.5194/gmd-14-495-2021, 2021
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Dry deposition to vegetation is a major sink of ground-level ozone. Its parameterization in atmospheric chemistry models represents a significant source of uncertainty for global tropospheric ozone. We extended the current model parameterization with a relevant pathway and important meteorological adjustment factors. The comparison with measurements shows that this enables a more realistic model representation of ozone dry deposition velocity. Globally, annual dry deposition loss increases.
Laura Stecher, Franziska Winterstein, Martin Dameris, Patrick Jöckel, Michael Ponater, and Markus Kunze
Atmos. Chem. Phys., 21, 731–754, https://doi.org/10.5194/acp-21-731-2021, https://doi.org/10.5194/acp-21-731-2021, 2021
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This study investigates the impact of strongly increased atmospheric methane mixing ratios on the Earth's climate. An interactive model system including atmospheric dynamics, chemistry, and a mixed-layer ocean model is used to analyse the effect of doubled and quintupled methane mixing ratios. We assess feedbacks on atmospheric chemistry and changes in the stratospheric circulation, focusing on the impact of tropospheric warming, and their relevance for the model's climate sensitivity.
Arseniy Karagodin-Doyennel, Eugene Rozanov, Ales Kuchar, William Ball, Pavle Arsenovic, Ellis Remsberg, Patrick Jöckel, Markus Kunze, David A. Plummer, Andrea Stenke, Daniel Marsh, Doug Kinnison, and Thomas Peter
Atmos. Chem. Phys., 21, 201–216, https://doi.org/10.5194/acp-21-201-2021, https://doi.org/10.5194/acp-21-201-2021, 2021
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The solar signal in the mesospheric H2O and CO was extracted from the CCMI-1 model simulations and satellite observations using multiple linear regression (MLR) analysis. MLR analysis shows a pronounced and statistically robust solar signal in both H2O and CO. The model results show a general agreement with observations reproducing a negative/positive solar signal in H2O/CO. The pattern of the solar signal varies among the considered models, reflecting some differences in the model setup.
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.
Edward J. Charlesworth, Ann-Kristin Dugstad, Frauke Fritsch, Patrick Jöckel, and Felix Plöger
Atmos. Chem. Phys., 20, 15227–15245, https://doi.org/10.5194/acp-20-15227-2020, https://doi.org/10.5194/acp-20-15227-2020, 2020
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Modeling the stratosphere requires models with good representations of chemical transport. To do this, nearly all models divide the atmosphere into boxes. This creates some unwanted problems. However, the only other option is to divide the atmosphere into balloons, and this method is very complicated. Here, we use a model which uses this balloon-like method to estimate the impacts of this method on chemical transport. We find significant differences in sensitive regions of the stratosphere.
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.
Yuanhong Zhao, Marielle Saunois, Philippe Bousquet, Xin Lin, Antoine Berchet, Michaela I. Hegglin, Josep G. Canadell, Robert B. Jackson, Makoto Deushi, Patrick Jöckel, Douglas Kinnison, Ole Kirner, Sarah Strode, Simone Tilmes, Edward J. Dlugokencky, and Bo Zheng
Atmos. Chem. Phys., 20, 13011–13022, https://doi.org/10.5194/acp-20-13011-2020, https://doi.org/10.5194/acp-20-13011-2020, 2020
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Decadal trends and variations in OH are critical for understanding atmospheric CH4 evolution. We quantify the impacts of OH trends and variations on the CH4 budget by conducting CH4 inversions on a decadal scale with an ensemble of OH fields. We find the negative OH anomalies due to enhanced fires can reduce the optimized CH4 emissions by up to 10 Tg yr−1 during El Niño years and the positive OH trend from 1986 to 2010 results in a ∼ 23 Tg yr−1 additional increase in optimized CH4 emissions.
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.
Alina Fiehn, Julian Kostinek, Maximilian Eckl, Theresa Klausner, Michał Gałkowski, Jinxuan Chen, Christoph Gerbig, Thomas Röckmann, Hossein Maazallahi, Martina Schmidt, Piotr Korbeń, Jarosław Neçki, Pawel Jagoda, Norman Wildmann, Christian Mallaun, Rostyslav Bun, Anna-Leah Nickl, Patrick Jöckel, Andreas Fix, and Anke Roiger
Atmos. Chem. Phys., 20, 12675–12695, https://doi.org/10.5194/acp-20-12675-2020, https://doi.org/10.5194/acp-20-12675-2020, 2020
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A severe reduction of greenhouse gas emissions is necessary to fulfill the Paris Agreement. We use aircraft- and ground-based in situ observations of trace gases and wind speed from two flights over the Upper Silesian Coal Basin, Poland, for independent emission estimation. The derived methane emission estimates are within the range of emission inventories, carbon dioxide estimates are in the lower range and carbon monoxide emission estimates are slightly higher than emission inventory values.
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.
Markus Kilian, Sabine Brinkop, and Patrick Jöckel
Atmos. Chem. Phys., 20, 11697–11715, https://doi.org/10.5194/acp-20-11697-2020, https://doi.org/10.5194/acp-20-11697-2020, 2020
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After the volcanic eruption of Mt Pinatubo in 1991, ozone decreased in the tropics and increased in the midlatitudes and polar regions for 1 year. The change in the ozone column is solely a result of the volcanic heating, followed by an ozone decrease in the higher latitudes. This is caused by the volcanic aerosol, which changes the heterogeneous chemistry and thus the catalytic ozone loss cycles. Vertical transport of water vapour is enhanced by volcanic heating and increases methane.
Hiroshi Yamashita, Feijia Yin, Volker Grewe, Patrick Jöckel, Sigrun Matthes, Bastian Kern, Katrin Dahlmann, and Christine Frömming
Geosci. Model Dev., 13, 4869–4890, https://doi.org/10.5194/gmd-13-4869-2020, https://doi.org/10.5194/gmd-13-4869-2020, 2020
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This paper describes the updated submodel AirTraf 2.0 which simulates global air traffic in the ECHAM/MESSy Atmospheric Chemistry (EMAC) model. Nine aircraft routing options have been integrated, including contrail avoidance, minimum economic costs, and minimum climate impact. Example simulations reveal characteristics of different routing options on air traffic performances. The consistency of the AirTraf simulations is verified with literature data.
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.
Matt Amos, Paul J. Young, J. Scott Hosking, Jean-François Lamarque, N. Luke Abraham, Hideharu Akiyoshi, Alexander T. Archibald, Slimane Bekki, Makoto Deushi, Patrick Jöckel, Douglas Kinnison, Ole Kirner, Markus Kunze, Marion Marchand, David A. Plummer, David Saint-Martin, Kengo Sudo, Simone Tilmes, and Yousuke Yamashita
Atmos. Chem. Phys., 20, 9961–9977, https://doi.org/10.5194/acp-20-9961-2020, https://doi.org/10.5194/acp-20-9961-2020, 2020
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We present an updated projection of Antarctic ozone hole recovery using an ensemble of chemistry–climate models. To do so, we employ a method, more advanced and skilful than the current multi-model mean standard, which is applicable to other ensemble analyses. It calculates the performance and similarity of the models, which we then use to weight the model. Calculating model similarity allows us to account for models which are constructed from similar components.
Mariano Mertens, Astrid Kerkweg, Volker Grewe, Patrick Jöckel, and Robert Sausen
Atmos. Chem. Phys., 20, 7843–7873, https://doi.org/10.5194/acp-20-7843-2020, https://doi.org/10.5194/acp-20-7843-2020, 2020
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We investigate the contribution of land transport emissions to ozone and ozone precursors in Europe and Germany. Our results show that land transport emissions are one of the most important contributors to reactive nitrogen in Europe. The contribution to ozone is in the range of 8 % to 16 % and varies strongly for different seasons. The hots-pots with the largest ozone concentrations are the Po Valley, while the largest concentration to reactive nitrogen is located mainly in western Europe.
Daniele Visioni, Giovanni Pitari, Vincenzo Rizi, Marco Iarlori, Irene Cionni, Ilaria Quaglia, Hideharu Akiyoshi, Slimane Bekki, Neal Butchart, Martin Chipperfield, Makoto Deushi, Sandip S. Dhomse, Rolando Garcia, Patrick Joeckel, Douglas Kinnison, Jean-François Lamarque, Marion Marchand, Martine Michou, Olaf Morgenstern, Tatsuya Nagashima, Fiona M. O'Connor, Luke D. Oman, David Plummer, Eugene Rozanov, David Saint-Martin, Robyn Schofield, John Scinocca, Andrea Stenke, Kane Stone, Kengo Sudo, Taichu Y. Tanaka, Simone Tilmes, Holger Tost, Yousuke Yamashita, and Guang Zeng
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-525, https://doi.org/10.5194/acp-2020-525, 2020
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In this work we analyse the trend in ozone profiles taken at L'Aquila (Italy, 42.4° N) for seventeen years, between 2000 and 2016 and compare them against already available measured ozone trends. We try to understand and explain the observed trends at various heights in light of the simulations from seventeen different model, highlighting the contribution of changes in circulation and chemical ozone loss during this time period.
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.
Marta Abalos, Clara Orbe, Douglas E. Kinnison, David Plummer, Luke D. Oman, Patrick Jöckel, Olaf Morgenstern, Rolando R. Garcia, Guang Zeng, Kane A. Stone, and Martin Dameris
Atmos. Chem. Phys., 20, 6883–6901, https://doi.org/10.5194/acp-20-6883-2020, https://doi.org/10.5194/acp-20-6883-2020, 2020
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A set of state-of-the art chemistry–climate models is used to examine future changes in downward transport from the stratosphere, a key contributor to tropospheric ozone. The acceleration of the stratospheric circulation results in increased stratosphere-to-troposphere transport. In the subtropics, downward advection into the troposphere is enhanced due to climate change. At higher latitudes, the ozone reservoir above the tropopause is enlarged due to the stronger circulation and ozone recovery.
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.
Simon Rosanka, Giang H. T. Vu, Hue M. T. Nguyen, Tien V. Pham, Umar Javed, Domenico Taraborrelli, and Luc Vereecken
Atmos. Chem. Phys., 20, 6671–6686, https://doi.org/10.5194/acp-20-6671-2020, https://doi.org/10.5194/acp-20-6671-2020, 2020
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Isocyanic acid, HNCO, is a toxic chemical compound emitted to the atmosphere by biomass burning and by unwanted release in NOx mitigation systems in vehicles such as the AdBlue system. We have studied the loss processes of HNCO, finding that it is unreactive to most atmospheric oxidants and thus has a long chemical lifetime. The main removal is then by deposition on surfaces and transition to aqueous phase, such as clouds. The long lifetime also allows it to be transported to the stratosphere.
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.
Anna-Leah Nickl, Mariano Mertens, Anke Roiger, Andreas Fix, Axel Amediek, Alina Fiehn, Christoph Gerbig, Michal Galkowski, Astrid Kerkweg, Theresa Klausner, Maximilian Eckl, and Patrick Jöckel
Geosci. Model Dev., 13, 1925–1943, https://doi.org/10.5194/gmd-13-1925-2020, https://doi.org/10.5194/gmd-13-1925-2020, 2020
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Based on the global and regional chemistry–climate model system MECO(n), we implemented a forecast system to support the planning of measurement campaign research flights with chemical weather forecasts. We applied this system for the first time to provide 6 d forecasts in support of the CoMet 1.0
campaign targeting methane emitted from coal mining ventilation shafts in the Upper Silesian Coal Basin in Poland. We describe the new forecast system and evaluate its forecast skill.
Timo Keber, Harald Bönisch, Carl Hartick, Marius Hauck, Fides Lefrancois, Florian Obersteiner, Akima Ringsdorf, Nils Schohl, Tanja Schuck, Ryan Hossaini, Phoebe Graf, Patrick Jöckel, and Andreas Engel
Atmos. Chem. Phys., 20, 4105–4132, https://doi.org/10.5194/acp-20-4105-2020, https://doi.org/10.5194/acp-20-4105-2020, 2020
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In this paper we summarize observations of short-lived halocarbons in the tropopause region. We show that, especially during winter, the levels of short-lived bromine gases at the extratropical tropopause are higher than at the tropical tropopause. We discuss the impact of the distributions on stratospheric bromine levels and compare our observations to two models with four different emission scenarios.
Clara Orbe, David A. Plummer, Darryn W. Waugh, Huang Yang, Patrick Jöckel, Douglas E. Kinnison, Beatrice Josse, Virginie Marecal, Makoto Deushi, Nathan Luke Abraham, Alexander T. Archibald, Martyn P. Chipperfield, Sandip Dhomse, Wuhu Feng, and Slimane Bekki
Atmos. Chem. Phys., 20, 3809–3840, https://doi.org/10.5194/acp-20-3809-2020, https://doi.org/10.5194/acp-20-3809-2020, 2020
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Atmospheric composition is strongly influenced by global-scale winds that are not always properly simulated in computer models. A common approach to correct for this bias is to relax or
nudgeto the observed winds. Here we systematically evaluate how well this technique performs across a large suite of chemistry–climate models in terms of its ability to reproduce key aspects of both the tropospheric and stratospheric circulations.
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.
Anna Novelli, Luc Vereecken, Birger Bohn, Hans-Peter Dorn, Georgios I. Gkatzelis, Andreas Hofzumahaus, Frank Holland, David Reimer, Franz Rohrer, Simon Rosanka, Domenico Taraborrelli, Ralf Tillmann, Robert Wegener, Zhujun Yu, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 20, 3333–3355, https://doi.org/10.5194/acp-20-3333-2020, https://doi.org/10.5194/acp-20-3333-2020, 2020
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Experimental evidence from a simulation chamber study shows that the regeneration efficiency of the hydroxyl radical is maintained globally at values higher than 0.5 for a wide range of nitrogen oxide concentrations as a result of isomerizations of peroxy radicals originating from the OH oxidation of isoprene. The available models were tested, and suggestions on how to improve their ability to reproduce the measured radical and oxygenated volatile organic compound concentrations are provided.
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.
Julie M. Nicely, Bryan N. Duncan, Thomas F. Hanisco, Glenn M. Wolfe, Ross J. Salawitch, Makoto Deushi, Amund S. Haslerud, Patrick Jöckel, Béatrice Josse, Douglas E. Kinnison, Andrew Klekociuk, Michael E. Manyin, Virginie Marécal, Olaf Morgenstern, Lee T. Murray, Gunnar Myhre, Luke D. Oman, Giovanni Pitari, Andrea Pozzer, Ilaria Quaglia, Laura E. Revell, Eugene Rozanov, Andrea Stenke, Kane Stone, Susan Strahan, Simone Tilmes, Holger Tost, Daniel M. Westervelt, and Guang Zeng
Atmos. Chem. Phys., 20, 1341–1361, https://doi.org/10.5194/acp-20-1341-2020, https://doi.org/10.5194/acp-20-1341-2020, 2020
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Differences in methane lifetime among global models are large and poorly understood. We use a neural network method and simulations from the Chemistry Climate Model Initiative to quantify the factors influencing methane lifetime spread among models and variations over time. UV photolysis, tropospheric ozone, and nitrogen oxides drive large model differences, while the same factors plus specific humidity contribute to a decreasing trend in methane lifetime between 1980 and 2015.
Mariano Mertens, Astrid Kerkweg, Volker Grewe, Patrick Jöckel, and Robert Sausen
Geosci. Model Dev., 13, 363–383, https://doi.org/10.5194/gmd-13-363-2020, https://doi.org/10.5194/gmd-13-363-2020, 2020
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This study investigates if ozone source apportionment results using a tagged tracer approach depend on the resolutions of the applied model and/or emission inventory. For this we apply a global to regional atmospheric chemistry model, which allows us to compare the results on global and regional scales. Our results show that differences on the continental scale (e.g. Europe) are rather small (10 %); on the regional scale, however, differences of up to 30 % were found.
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.
Le Kuai, Kevin W. Bowman, Kazuyuki Miyazaki, Makoto Deushi, Laura Revell, Eugene Rozanov, Fabien Paulot, Sarah Strode, Andrew Conley, Jean-François Lamarque, Patrick Jöckel, David A. Plummer, Luke D. Oman, Helen Worden, Susan Kulawik, David Paynter, Andrea Stenke, and Markus Kunze
Atmos. Chem. Phys., 20, 281–301, https://doi.org/10.5194/acp-20-281-2020, https://doi.org/10.5194/acp-20-281-2020, 2020
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The tropospheric ozone increase from pre-industrial to the present day leads to a radiative forcing. The top-of-atmosphere outgoing fluxes at the ozone band are controlled by ozone, water vapor, and temperature. We demonstrate a method to attribute the models’ flux biases to these key players using satellite-constrained instantaneous radiative kernels. The largest spread between models is found in the tropics, mainly driven by ozone and then water vapor.
Dimitris Akritidis, Andrea Pozzer, and Prodromos Zanis
Atmos. Chem. Phys., 19, 14387–14401, https://doi.org/10.5194/acp-19-14387-2019, https://doi.org/10.5194/acp-19-14387-2019, 2019
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We investigate the impact of future climate change under the RCP6.0 scenario on tropopause folds and tropospheric ozone, using a transient EMAC simulation and a tropopause fold detection algorithm. A strengthening of ozone stratosphere-to-troposphere transport (STT) is projected for the future, resulting in an increase in upper- and middle-tropospheric ozone. The maxima of future ozone STT increases are mainly projected for regions where tropopause folds are expected to occur more frequently.
Martin Dameris, Patrick Jöckel, and Matthias Nützel
Atmos. Chem. Phys., 19, 13759–13771, https://doi.org/10.5194/acp-19-13759-2019, https://doi.org/10.5194/acp-19-13759-2019, 2019
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A chemistry–climate model (CCM) study is performed, investigating the consequences of a constant CFC-11 surface mixing ratio for stratospheric ozone in the future. The total column ozone is particularly affected in both polar regions in winter and spring. It turns out that the calculated ozone changes, especially in the upper stratosphere, are smaller than expected. In this attitudinal region the additional ozone depletion due to the catalysis by reactive chlorine is partly compensated for.
Yuanhong Zhao, Marielle Saunois, Philippe Bousquet, Xin Lin, Antoine Berchet, Michaela I. Hegglin, Josep G. Canadell, Robert B. Jackson, Didier A. Hauglustaine, Sophie Szopa, Ann R. Stavert, Nathan Luke Abraham, Alex T. Archibald, Slimane Bekki, Makoto Deushi, Patrick Jöckel, Béatrice Josse, Douglas Kinnison, Ole Kirner, Virginie Marécal, Fiona M. O'Connor, David A. Plummer, Laura E. Revell, Eugene Rozanov, Andrea Stenke, Sarah Strode, Simone Tilmes, Edward J. Dlugokencky, and Bo Zheng
Atmos. Chem. Phys., 19, 13701–13723, https://doi.org/10.5194/acp-19-13701-2019, https://doi.org/10.5194/acp-19-13701-2019, 2019
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The role of hydroxyl radical changes in methane trends is debated, hindering our understanding of the methane cycle. This study quantifies how uncertainties in the hydroxyl radical may influence methane abundance in the atmosphere based on the inter-model comparison of hydroxyl radical fields and model simulations of CH4 abundance with different hydroxyl radical scenarios during 2000–2016. We show that hydroxyl radical changes could contribute up to 54 % of model-simulated methane biases.
Andreas Luther, Ralph Kleinschek, Leon Scheidweiler, Sara Defratyka, Mila Stanisavljevic, Andreas Forstmaier, Alexandru Dandocsi, Sebastian Wolff, Darko Dubravica, Norman Wildmann, Julian Kostinek, Patrick Jöckel, Anna-Leah Nickl, Theresa Klausner, Frank Hase, Matthias Frey, Jia Chen, Florian Dietrich, Jarosław Nȩcki, Justyna Swolkień, Andreas Fix, Anke Roiger, and André Butz
Atmos. Meas. Tech., 12, 5217–5230, https://doi.org/10.5194/amt-12-5217-2019, https://doi.org/10.5194/amt-12-5217-2019, 2019
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Methane ventilated from hard coal mines in the Upper Silesian
Coal Basin in Poland is measured with a mobile Fourier transform spectrometer EM27/SUN. The instrument was mounted on a truck driving in stop-and-go patterns downwind of the methane sources. The emissions are estimated with the cross-sectional flux method. Calculated emissions are in broad agreement with the E-PRTR database. Wind-related errors on the methane estimates dominate the error budget and typically amount to 20 %.
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.
Andreas Chrysanthou, Amanda C. Maycock, Martyn P. Chipperfield, Sandip Dhomse, Hella Garny, Douglas Kinnison, Hideharu Akiyoshi, Makoto Deushi, Rolando R. Garcia, Patrick Jöckel, Oliver Kirner, Giovanni Pitari, David A. Plummer, Laura Revell, Eugene Rozanov, Andrea Stenke, Taichu Y. Tanaka, Daniele Visioni, and Yousuke Yamashita
Atmos. Chem. Phys., 19, 11559–11586, https://doi.org/10.5194/acp-19-11559-2019, https://doi.org/10.5194/acp-19-11559-2019, 2019
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We perform the first multi-model comparison of the impact of nudged meteorology on the stratospheric residual circulation (RC) in chemistry–climate models. Nudging meteorology does not constrain the mean strength of RC compared to free-running simulations, and despite the lack of agreement in the mean circulation, nudging tightly constrains the inter-annual variability in the tropical upward mass flux in the lower stratosphere. In summary, nudging strongly affects the representation of RC.
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.
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.
Kévin Lamy, Thierry Portafaix, Béatrice Josse, Colette Brogniez, Sophie Godin-Beekmann, Hassan Bencherif, Laura Revell, Hideharu Akiyoshi, Slimane Bekki, Michaela I. Hegglin, Patrick Jöckel, Oliver Kirner, Ben Liley, Virginie Marecal, Olaf Morgenstern, Andrea Stenke, Guang Zeng, N. Luke Abraham, Alexander T. Archibald, Neil Butchart, Martyn P. Chipperfield, Glauco Di Genova, Makoto Deushi, Sandip S. Dhomse, Rong-Ming Hu, Douglas Kinnison, Michael Kotkamp, Richard McKenzie, Martine Michou, Fiona M. O'Connor, Luke D. Oman, Giovanni Pitari, David A. Plummer, John A. Pyle, Eugene Rozanov, David Saint-Martin, Kengo Sudo, Taichu Y. Tanaka, Daniele Visioni, and Kohei Yoshida
Atmos. Chem. Phys., 19, 10087–10110, https://doi.org/10.5194/acp-19-10087-2019, https://doi.org/10.5194/acp-19-10087-2019, 2019
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In this study, we simulate the ultraviolet radiation evolution during the 21st century on Earth's surface using the output from several numerical models which participated in the Chemistry-Climate Model Initiative. We present four possible futures which depend on greenhouse gases emissions. The role of ozone-depleting substances, greenhouse gases and aerosols are investigated. Our results emphasize the important role of aerosols for future ultraviolet radiation in the Northern Hemisphere.
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.
Ohad Harari, Chaim I. Garfinkel, Shlomi Ziskin Ziv, Olaf Morgenstern, Guang Zeng, Simone Tilmes, Douglas Kinnison, Makoto Deushi, Patrick Jöckel, Andrea Pozzer, Fiona M. O'Connor, and Sean Davis
Atmos. Chem. Phys., 19, 9253–9268, https://doi.org/10.5194/acp-19-9253-2019, https://doi.org/10.5194/acp-19-9253-2019, 2019
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Ozone depletion in the Antarctic has been shown to influence surface conditions, but the effects of ozone depletion in the Arctic on surface climate are unclear. We show that Arctic ozone does influence surface climate in both polar regions and tropical regions, though the proximate cause of these surface impacts is not yet clear.
Petr Šácha, Roland Eichinger, Hella Garny, Petr Pišoft, Simone Dietmüller, Laura de la Torre, David A. Plummer, Patrick Jöckel, Olaf Morgenstern, Guang Zeng, Neal Butchart, and Juan A. Añel
Atmos. Chem. Phys., 19, 7627–7647, https://doi.org/10.5194/acp-19-7627-2019, https://doi.org/10.5194/acp-19-7627-2019, 2019
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Climate models robustly project a Brewer–Dobson circulation (BDC) acceleration in the course of climate change. Analyzing mean age of stratospheric air (AoA) from a subset of climate projection simulations, we find a remarkable agreement in simulating the largest AoA trends in the extratropical stratosphere. This is shown to be related with the upward shift of the circulation, resulting in a so-called stratospheric shrinkage, which could be one of the so-far-omitted BDC acceleration drivers.
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.
Franziska Winterstein, Fabian Tanalski, Patrick Jöckel, Martin Dameris, and Michael Ponater
Atmos. Chem. Phys., 19, 7151–7163, https://doi.org/10.5194/acp-19-7151-2019, https://doi.org/10.5194/acp-19-7151-2019, 2019
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The atmospheric concentrations of the anthropogenic greenhouse gas methane are predicted to rise in the future. In this paper we investigate how very strong methane concentrations will impact the atmosphere. We analyse two experiments, one with doubled and one with quintupled methane concentrations and focus on the rapid atmospheric changes before the ocean adjusts to the induced
forcing. In particular these are changes in temperature, ozone, the hydroxyl radical and stratospheric water vapour.
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.
Sabine Brinkop and Patrick Jöckel
Geosci. Model Dev., 12, 1991–2008, https://doi.org/10.5194/gmd-12-1991-2019, https://doi.org/10.5194/gmd-12-1991-2019, 2019
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We have extended ATTILA (Atmospheric Tracer Transport in a LAgrangian model), a Lagrangian tracer transport scheme which is online coupled to the global ECHAM/MESSy Atmospheric Chemistry (EMAC) model, with a combination of newly developed and modified physical routines and new diagnostic and infrastructure submodels. The results show an improvement of the tracer transport into and within the stratosphere due to the newly implemented diabatic vertical velocity.
Vincent Huijnen, Andrea Pozzer, Joaquim Arteta, Guy Brasseur, Idir Bouarar, Simon Chabrillat, Yves Christophe, Thierno Doumbia, Johannes Flemming, Jonathan Guth, Béatrice Josse, Vlassis A. Karydis, Virginie Marécal, and Sophie Pelletier
Geosci. Model Dev., 12, 1725–1752, https://doi.org/10.5194/gmd-12-1725-2019, https://doi.org/10.5194/gmd-12-1725-2019, 2019
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We report on an evaluation of tropospheric ozone and its precursor gases in three atmospheric chemistry versions as implemented in ECMWF’s Integrated Forecasting System (IFS), referred to as IFS(CB05BASCOE), IFS(MOZART) and IFS(MOCAGE). This configuration of having various chemistry versions within IFS provides a quantification of uncertainties in CAMS trace gas products that are induced by chemistry modelling.
Huang Yang, Darryn W. Waugh, Clara Orbe, Guang Zeng, Olaf Morgenstern, Douglas E. Kinnison, Jean-Francois Lamarque, Simone Tilmes, David A. Plummer, Patrick Jöckel, Susan E. Strahan, Kane A. Stone, and Robyn Schofield
Atmos. Chem. Phys., 19, 5511–5528, https://doi.org/10.5194/acp-19-5511-2019, https://doi.org/10.5194/acp-19-5511-2019, 2019
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We evaluate the performance of a suite of models in simulating the large-scale transport from the northern midlatitudes to the Arctic using a CO-like idealized tracer. We find a large multi-model spread of the Arctic concentration of this CO-like tracer that is well correlated with the differences in the location of the midlatitude jet as well as the northern Hadley Cell edge. Our results suggest the Hadley Cell is key and zonal-mean transport by surface meridional flow needs better constraint.
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.
Ryan S. Williams, Michaela I. Hegglin, Brian J. Kerridge, Patrick Jöckel, Barry G. Latter, and David A. Plummer
Atmos. Chem. Phys., 19, 3589–3620, https://doi.org/10.5194/acp-19-3589-2019, https://doi.org/10.5194/acp-19-3589-2019, 2019
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Tropospheric ozone has important implications for air quality and climate change but is poorly understood at a regional and seasonal level. Analysis of model simulations indicates that downward transport of ozone from the stratosphere has a larger influence than previously thought (as much as ~50 % even near the surface). Recent estimated changes in tropospheric ozone (1980–89 to 2001–10) are generally positive, with substantial attribution from the stratosphere identified over some regions.
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.
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.
J. Christopher Kaiser, Johannes Hendricks, Mattia Righi, Patrick Jöckel, Holger Tost, Konrad Kandler, Bernadett Weinzierl, Daniel Sauer, Katharina Heimerl, Joshua P. Schwarz, Anne E. Perring, and Thomas Popp
Geosci. Model Dev., 12, 541–579, https://doi.org/10.5194/gmd-12-541-2019, https://doi.org/10.5194/gmd-12-541-2019, 2019
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The implementation of the aerosol microphysics submodel MADE3 into the global atmospheric chemistry model EMAC is described and evaluated against an extensive pool of observational data, focusing on aerosol mass and number concentrations, size distributions, composition, and optical properties. EMAC (MADE3) is able to reproduce main aerosol properties reasonably well, in line with the performance of other global aerosol models.
Roland Eichinger, Simone Dietmüller, Hella Garny, Petr Šácha, Thomas Birner, Harald Bönisch, Giovanni Pitari, Daniele Visioni, Andrea Stenke, Eugene Rozanov, Laura Revell, David A. Plummer, Patrick Jöckel, Luke Oman, Makoto Deushi, Douglas E. Kinnison, Rolando Garcia, Olaf Morgenstern, Guang Zeng, Kane Adam Stone, and Robyn Schofield
Atmos. Chem. Phys., 19, 921–940, https://doi.org/10.5194/acp-19-921-2019, https://doi.org/10.5194/acp-19-921-2019, 2019
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To shed more light upon the changes in stratospheric circulation in the 21st century, climate projection simulations of 10 state-of-the-art global climate models, spanning from 1960 to 2100, are analyzed. The study shows that in addition to changes in transport, mixing also plays an important role in stratospheric circulation and that the properties of mixing vary over time. Furthermore, the influence of mixing is quantified and a dynamical framework is provided to understand the changes.
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
Laura E. Revell, Andrea Stenke, Fiona Tummon, Aryeh Feinberg, Eugene Rozanov, Thomas Peter, N. Luke Abraham, Hideharu Akiyoshi, Alexander T. Archibald, Neal Butchart, Makoto Deushi, Patrick Jöckel, Douglas Kinnison, Martine Michou, Olaf Morgenstern, Fiona M. O'Connor, Luke D. Oman, Giovanni Pitari, David A. Plummer, Robyn Schofield, Kane Stone, Simone Tilmes, Daniele Visioni, Yousuke Yamashita, and Guang Zeng
Atmos. Chem. Phys., 18, 16155–16172, https://doi.org/10.5194/acp-18-16155-2018, https://doi.org/10.5194/acp-18-16155-2018, 2018
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Global models such as those participating in the Chemistry-Climate Model Initiative (CCMI) consistently simulate biases in tropospheric ozone compared with observations. We performed an advanced statistical analysis with one of the CCMI models to understand the cause of the bias. We found that emissions of ozone precursor gases are the dominant driver of the bias, implying either that the emissions are too large, or that the way in which the model handles emissions needs to be improved.
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.
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.
Amanda C. Maycock, Katja Matthes, Susann Tegtmeier, Hauke Schmidt, Rémi Thiéblemont, Lon Hood, Hideharu Akiyoshi, Slimane Bekki, Makoto Deushi, Patrick Jöckel, Oliver Kirner, Markus Kunze, Marion Marchand, Daniel R. Marsh, Martine Michou, David Plummer, Laura E. Revell, Eugene Rozanov, Andrea Stenke, Yousuke Yamashita, and Kohei Yoshida
Atmos. Chem. Phys., 18, 11323–11343, https://doi.org/10.5194/acp-18-11323-2018, https://doi.org/10.5194/acp-18-11323-2018, 2018
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The 11-year solar cycle is an important driver of climate variability. Changes in incoming solar ultraviolet radiation affect atmospheric ozone, which in turn influences atmospheric temperatures. Constraining the impact of the solar cycle on ozone is therefore important for understanding climate variability. This study examines the representation of the solar influence on ozone in numerical models used to simulate past and future climate. We highlight important differences among model datasets.
Scarlet Stadtler, Thomas Kühn, Sabine Schröder, Domenico Taraborrelli, Martin G. Schultz, and Harri Kokkola
Geosci. Model Dev., 11, 3235–3260, https://doi.org/10.5194/gmd-11-3235-2018, https://doi.org/10.5194/gmd-11-3235-2018, 2018
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Atmospheric aerosols interact with our climate system and have adverse health effects. Nevertheless, these particles are a source of uncertainty in climate projections and the formation process of secondary aerosols formed by organic gas-phase precursors is particularly not fully understood. In order to gain a deeper understanding of secondary organic aerosol formation, this model system explicitly represents gas-phase and aerosol formation processes. Finally, this allows for process discussion.
Blanca Ayarzagüena, Lorenzo M. Polvani, Ulrike Langematz, Hideharu Akiyoshi, Slimane Bekki, Neal Butchart, Martin Dameris, Makoto Deushi, Steven C. Hardiman, Patrick Jöckel, Andrew Klekociuk, Marion Marchand, Martine Michou, Olaf Morgenstern, Fiona M. O'Connor, Luke D. Oman, David A. Plummer, Laura Revell, Eugene Rozanov, David Saint-Martin, John Scinocca, Andrea Stenke, Kane Stone, Yousuke Yamashita, Kohei Yoshida, and Guang Zeng
Atmos. Chem. Phys., 18, 11277–11287, https://doi.org/10.5194/acp-18-11277-2018, https://doi.org/10.5194/acp-18-11277-2018, 2018
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Stratospheric sudden warmings (SSWs) are natural major disruptions of the polar stratospheric circulation that also affect surface weather. In the literature there are conflicting claims as to whether SSWs will change in the future. The confusion comes from studies using different models and methods. Here we settle the question by analysing 12 models with a consistent methodology, to show that no robust changes in frequency and other features are expected over the 21st century.
Maarten Krol, Marco de Bruine, Lars Killaars, Huug Ouwersloot, Andrea Pozzer, Yi Yin, Frederic Chevallier, Philippe Bousquet, Prabir Patra, Dmitry Belikov, Shamil Maksyutov, Sandip Dhomse, Wuhu Feng, and Martyn P. Chipperfield
Geosci. Model Dev., 11, 3109–3130, https://doi.org/10.5194/gmd-11-3109-2018, https://doi.org/10.5194/gmd-11-3109-2018, 2018
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The TransCom inter-comparison project regularly carries out studies to quantify errors in simulated atmospheric transport. This paper presents the first results of an age of air (AoA) inter-comparison of six global transport models. Following a protocol, six models simulated five tracers from which atmospheric transport times can easily be deduced. Results highlight that inter-model differences associated with atmospheric transport are still large and require further analysis.
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.
Franziska Frank, Patrick Jöckel, Sergey Gromov, and Martin Dameris
Atmos. Chem. Phys., 18, 9955–9973, https://doi.org/10.5194/acp-18-9955-2018, https://doi.org/10.5194/acp-18-9955-2018, 2018
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It is frequently assumed that one methane molecule produces two water molecules. Applying various modeling concepts, we find that the yield of water from methane is vertically not constantly 2. In the upper stratosphere and lower mesosphere, transport of intermediate H2 molecules even led to a yield greater than 2. We conclude that for a realistic chemical source of stratospheric water vapor, one must also take other sources (H2), intermediates and the chemical removal of water into account.
Sergey Gromov, Carl A. M. Brenninkmeijer, and Patrick Jöckel
Atmos. Chem. Phys., 18, 9831–9843, https://doi.org/10.5194/acp-18-9831-2018, https://doi.org/10.5194/acp-18-9831-2018, 2018
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Using the observational data on 13C (CO) and 13C (CH4) from the extra-tropical Southern Hemisphere (ETSH) and EMAC model we (1) provide an independent, observation-based evaluation of Cl atom concentration variations in the ETSH throughout 1994–2000, (2) show that the role of tropospheric Cl as a sink of CH4 is seriously overestimated in the literature, (3) demonstrate that the 13C/12C ratio of CO is a sensitive indicator for the isotopic composition of reacted CH4 and therefore for its sources.
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.
Sandip S. Dhomse, Douglas Kinnison, Martyn P. Chipperfield, Ross J. Salawitch, Irene Cionni, Michaela I. Hegglin, N. Luke Abraham, Hideharu Akiyoshi, Alex T. Archibald, Ewa M. Bednarz, Slimane Bekki, Peter Braesicke, Neal Butchart, Martin Dameris, Makoto Deushi, Stacey Frith, Steven C. Hardiman, Birgit Hassler, Larry W. Horowitz, Rong-Ming Hu, Patrick Jöckel, Beatrice Josse, Oliver Kirner, Stefanie Kremser, Ulrike Langematz, Jared Lewis, Marion Marchand, Meiyun Lin, Eva Mancini, Virginie Marécal, Martine Michou, Olaf Morgenstern, Fiona M. O'Connor, Luke Oman, Giovanni Pitari, David A. Plummer, John A. Pyle, Laura E. Revell, Eugene Rozanov, Robyn Schofield, Andrea Stenke, Kane Stone, Kengo Sudo, Simone Tilmes, Daniele Visioni, Yousuke Yamashita, and Guang Zeng
Atmos. Chem. Phys., 18, 8409–8438, https://doi.org/10.5194/acp-18-8409-2018, https://doi.org/10.5194/acp-18-8409-2018, 2018
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We analyse simulations from the Chemistry-Climate Model Initiative (CCMI) to estimate the return dates of the stratospheric ozone layer from depletion by anthropogenic chlorine and bromine. The simulations from 20 models project that global column ozone will return to 1980 values in 2047 (uncertainty range 2042–2052). Return dates in other regions vary depending on factors related to climate change and importance of chlorine and bromine. Column ozone in the tropics may continue to decline.
Stefan Lossow, Dale F. Hurst, Karen H. Rosenlof, Gabriele P. Stiller, Thomas von Clarmann, Sabine Brinkop, Martin Dameris, Patrick Jöckel, Doug E. Kinnison, Johannes Plieninger, David A. Plummer, Felix Ploeger, William G. Read, Ellis E. Remsberg, James M. Russell, and Mengchu Tao
Atmos. Chem. Phys., 18, 8331–8351, https://doi.org/10.5194/acp-18-8331-2018, https://doi.org/10.5194/acp-18-8331-2018, 2018
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Trend estimates of lower stratospheric H2O derived from the FPH observations at Boulder and a merged zonal mean satellite data set clearly differ for the time period from the late 1980s to 2010. We investigate if a sampling bias between Boulder and the zonal mean around the Boulder latitude can explain these trend discrepancies. Typically they are small and not sufficient to explain the trend discrepancies in the observational database.
Stefanie Meul, Ulrike Langematz, Philipp Kröger, Sophie Oberländer-Hayn, and Patrick Jöckel
Atmos. Chem. Phys., 18, 7721–7738, https://doi.org/10.5194/acp-18-7721-2018, https://doi.org/10.5194/acp-18-7721-2018, 2018
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Using a chemistry--climate model future changes in the stratosphere-to-troposphere ozone mass flux, their drivers, and the future distribution of stratospheric ozone in the troposphere are investigated. In an extreme greenhouse gas (GHG) scenario, the global influx of stratospheric ozone into the troposphere is projected to grow between 2000 and 2100 by 53%. The increase is due to the recovery of stratospheric ozone owing to declining halogens and GHG induced circulation and temperature changes.
Clara Orbe, Huang Yang, Darryn W. Waugh, Guang Zeng, Olaf Morgenstern, Douglas E. Kinnison, Jean-Francois Lamarque, Simone Tilmes, David A. Plummer, John F. Scinocca, Beatrice Josse, Virginie Marecal, Patrick Jöckel, Luke D. Oman, Susan E. Strahan, Makoto Deushi, Taichu Y. Tanaka, Kohei Yoshida, Hideharu Akiyoshi, Yousuke Yamashita, Andreas Stenke, Laura Revell, Timofei Sukhodolov, Eugene Rozanov, Giovanni Pitari, Daniele Visioni, Kane A. Stone, Robyn Schofield, and Antara Banerjee
Atmos. Chem. Phys., 18, 7217–7235, https://doi.org/10.5194/acp-18-7217-2018, https://doi.org/10.5194/acp-18-7217-2018, 2018
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In this study we compare a few atmospheric transport properties among several numerical models that are used to study the influence of atmospheric chemistry on climate. We show that there are large differences among models in terms of the timescales that connect the Northern Hemisphere midlatitudes, where greenhouse gases and ozone-depleting substances are emitted, to the Southern Hemisphere. Our results may have important implications for how models represent atmospheric composition.
Simone Dietmüller, Roland Eichinger, Hella Garny, Thomas Birner, Harald Boenisch, Giovanni Pitari, Eva Mancini, Daniele Visioni, Andrea Stenke, Laura Revell, Eugene Rozanov, David A. Plummer, John Scinocca, Patrick Jöckel, Luke Oman, Makoto Deushi, Shibata Kiyotaka, Douglas E. Kinnison, Rolando Garcia, Olaf Morgenstern, Guang Zeng, Kane Adam Stone, and Robyn Schofield
Atmos. Chem. Phys., 18, 6699–6720, https://doi.org/10.5194/acp-18-6699-2018, https://doi.org/10.5194/acp-18-6699-2018, 2018
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
Martin G. Schultz, Scarlet Stadtler, Sabine Schröder, Domenico Taraborrelli, Bruno Franco, Jonathan Krefting, Alexandra Henrot, Sylvaine Ferrachat, Ulrike Lohmann, David Neubauer, Colombe Siegenthaler-Le Drian, Sebastian Wahl, Harri Kokkola, Thomas Kühn, Sebastian Rast, Hauke Schmidt, Philip Stier, Doug Kinnison, Geoffrey S. Tyndall, John J. Orlando, and Catherine Wespes
Geosci. Model Dev., 11, 1695–1723, https://doi.org/10.5194/gmd-11-1695-2018, https://doi.org/10.5194/gmd-11-1695-2018, 2018
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The chemistry–climate model ECHAM-HAMMOZ contains a detailed representation of tropospheric and stratospheric reactive chemistry and state-of-the-art parameterizations of aerosols. It thus allows for detailed investigations of chemical processes in the climate system. Evaluation of the model with various observational data yields good results, but the model has a tendency to produce too much OH in the tropics. This highlights the important interplay between atmospheric chemistry and dynamics.
Klaus-Dirk Gottschaldt, Hans Schlager, Robert Baumann, Duy Sinh Cai, Veronika Eyring, Phoebe Graf, Volker Grewe, Patrick Jöckel, Tina Jurkat-Witschas, Christiane Voigt, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 18, 5655–5675, https://doi.org/10.5194/acp-18-5655-2018, https://doi.org/10.5194/acp-18-5655-2018, 2018
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This study places aircraft trace gas measurements from within the Asian summer monsoon anticyclone into the context of regional, intra- and interannual variability. We find that the processes reflected in the measurements are present throughout multiple simulated monsoon seasons. Dynamical instabilities, photochemical ozone production, lightning and entrainments from the lower troposphere and from the tropopause region determine the distinct composition of the anticyclone and its outflow.
Mariano Mertens, Volker Grewe, Vanessa S. Rieger, and Patrick Jöckel
Atmos. Chem. Phys., 18, 5567–5588, https://doi.org/10.5194/acp-18-5567-2018, https://doi.org/10.5194/acp-18-5567-2018, 2018
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We quantified the contribution of land transport and shipping emissions to tropospheric ozone using a global chemistry–climate model. Our results indicate a contribution to ground-level ozone from land transport emissions of up to 18 % in North America and Southern Europe as well as a contribution from shipping emissions of up to 30 % in the Pacific. Our estimates of the radiative ozone forcing due to land transport and shipping emissions are 92 mW m−2 and 62 mW m−2, respectively.
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.
Astrid Kerkweg, Christiane Hofmann, Patrick Jöckel, Mariano Mertens, and Gregor Pante
Geosci. Model Dev., 11, 1059–1076, https://doi.org/10.5194/gmd-11-1059-2018, https://doi.org/10.5194/gmd-11-1059-2018, 2018
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As part of the model documentation of the MECO(n) system, this article documents the basics of the Multi-Model-Driver expansion (MMD v2.0) to two-way coupling and the newly developed generic MESSy submodel GRID (v1.0), which is used by MMD v2.0 for the generalised definition of arbitrary grids and for the
transformation of data between them.
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.
Scarlet Stadtler, David Simpson, Sabine Schröder, Domenico Taraborrelli, Andreas Bott, and Martin Schultz
Atmos. Chem. Phys., 18, 3147–3171, https://doi.org/10.5194/acp-18-3147-2018, https://doi.org/10.5194/acp-18-3147-2018, 2018
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.
Andreas Engel, Harald Bönisch, Jennifer Ostermöller, Martyn P. Chipperfield, Sandip Dhomse, and Patrick Jöckel
Atmos. Chem. Phys., 18, 601–619, https://doi.org/10.5194/acp-18-601-2018, https://doi.org/10.5194/acp-18-601-2018, 2018
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We present a new method to derive equivalent effective stratospheric chlorine (EESC), which is based on an improved formulation of the propagation of trends of species with chemical loss from the troposphere to the stratosphere. EESC calculated with the new method shows much better agreement with model-derived ESC. Based on this new formulation, we expect the halogen impact on midlatitude stratospheric ozone to return to 1980 values about 10 years later, then using the current formulation.
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
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.
Tilman Hüneke, Oliver-Alex Aderhold, Jannik Bounin, Marcel Dorf, Eric Gentry, Katja Grossmann, Jens-Uwe Grooß, Peter Hoor, Patrick Jöckel, Mareike Kenntner, Marvin Knapp, Matthias Knecht, Dominique Lörks, Sabrina Ludmann, Sigrun Matthes, Rasmus Raecke, Marcel Reichert, Jannis Weimar, Bodo Werner, Andreas Zahn, Helmut Ziereis, and Klaus Pfeilsticker
Atmos. Meas. Tech., 10, 4209–4234, https://doi.org/10.5194/amt-10-4209-2017, https://doi.org/10.5194/amt-10-4209-2017, 2017
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This paper describes a novel instrument for the aircraft-borne remote sensing of trace gases and liquid and solid water. Until recently, such measurements could only be evaluated under clear-sky conditions. We present a characterization and error assessment of the novel "scaling method", which allows for the retrieval of absolute trace gas concentrations under all sky conditions, significantly expanding the applicability of such measurements to study atmospheric photochemistry.
Huisheng Bian, Mian Chin, Didier A. Hauglustaine, Michael Schulz, Gunnar Myhre, Susanne E. Bauer, Marianne T. Lund, Vlassis A. Karydis, Tom L. Kucsera, Xiaohua Pan, Andrea Pozzer, Ragnhild B. Skeie, Stephen D. Steenrod, Kengo Sudo, Kostas Tsigaridis, Alexandra P. Tsimpidi, and Svetlana G. Tsyro
Atmos. Chem. Phys., 17, 12911–12940, https://doi.org/10.5194/acp-17-12911-2017, https://doi.org/10.5194/acp-17-12911-2017, 2017
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Atmospheric nitrate contributes notably to total aerosol mass in the present day and is likely to be more important over the next century, with a projected decline in SO2 and NOx emissions and increase in NH3 emissions. This paper investigates atmospheric nitrate using multiple global models and measurements. The study is part of the AeroCom phase III activity. The study is the first attempt to look at global atmospheric nitrate simulation at physical and chemical process levels.
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.
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.
Stefan Lossow, Hella Garny, and Patrick Jöckel
Atmos. Chem. Phys., 17, 11521–11539, https://doi.org/10.5194/acp-17-11521-2017, https://doi.org/10.5194/acp-17-11521-2017, 2017
Stefanie Falk, Björn-Martin Sinnhuber, Gisèle Krysztofiak, Patrick Jöckel, Phoebe Graf, and Sinikka T. Lennartz
Atmos. Chem. Phys., 17, 11313–11329, https://doi.org/10.5194/acp-17-11313-2017, https://doi.org/10.5194/acp-17-11313-2017, 2017
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Brominated very short-lived source gases (VSLS) contribute significantly to the tropospheric and stratospheric bromine loading. We find an increase of future ocean–atmosphere flux of brominated VSLS of 8–10 % compared to present day. A decrease in the tropospheric mixing ratios of VSLS and an increase in the lower stratosphere are attributed to changes in atmospheric chemistry and transport. Bromine impact on stratospheric ozone at the end of the 21st century is reduced compared to present day.
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.
Sergey Gromov, Carl A. M. Brenninkmeijer, and Patrick Jöckel
Atmos. Chem. Phys., 17, 8525–8552, https://doi.org/10.5194/acp-17-8525-2017, https://doi.org/10.5194/acp-17-8525-2017, 2017
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We revisit the proxies/uncertainties for the 13C/12C ratios of emissions of reactive C into the atmosphere. Our main findings are (i) a factor of 2 less uncertain estimate of tropospheric CO surface sources δ13C, (ii) a confirmed disagreement between the bottom-up and top-down 13CO-inclusive emission estimates, and (iii) a novel estimate of the δ13C signatures of a range of NMHCs/VOCs to be used in modelling studies. Results are based on the EMAC model emission set-up evaluated for 2000.
Volker Grewe, Eleni Tsati, Mariano Mertens, Christine Frömming, and Patrick Jöckel
Geosci. Model Dev., 10, 2615–2633, https://doi.org/10.5194/gmd-10-2615-2017, https://doi.org/10.5194/gmd-10-2615-2017, 2017
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We present a diagnostics, implemented in an Earth system model, which keeps track of the contribution of source categories (mainly emission sectors) to various concentrations (O3 and HOx). For the first time, it takes into account chemically competing effects, e.g., the competition between ozone precursors in the production of ozone. We show that the results are in-line with results from other tagging schemes and provide plausibility checks for OH and HO2, which have not previously been tagged.
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.
Simone Dietmüller, Hella Garny, Felix Plöger, Patrick Jöckel, and Duy Cai
Atmos. Chem. Phys., 17, 7703–7719, https://doi.org/10.5194/acp-17-7703-2017, https://doi.org/10.5194/acp-17-7703-2017, 2017
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.
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.
Klaus-D. Gottschaldt, Hans Schlager, Robert Baumann, Heiko Bozem, Veronika Eyring, Peter Hoor, Patrick Jöckel, Tina Jurkat, Christiane Voigt, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 17, 6091–6111, https://doi.org/10.5194/acp-17-6091-2017, https://doi.org/10.5194/acp-17-6091-2017, 2017
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We present upper-tropospheric trace gas measurements in the Asian summer monsoon anticyclone, obtained with the HALO research aircraft in September 2012. The anticyclone is one of the largest atmospheric features on Earth, but many aspects of it are not well understood. With the help of model simulations we find that entrainments from the tropopause region and the lower troposphere, combined with photochemistry and dynamical instabilities, can explain the observations.
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.
Jennifer Ostermöller, Harald Bönisch, Patrick Jöckel, and Andreas Engel
Atmos. Chem. Phys., 17, 3785–3797, https://doi.org/10.5194/acp-17-3785-2017, https://doi.org/10.5194/acp-17-3785-2017, 2017
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We analysed the temporal evolution of fractional release factors (FRFs) from EMAC model simulations for several halocarbons and nitrous oxide. The current formulation of FRFs yields values that depend on the tropospheric trend of the species. This is a problematic issue for the application of FRF in the calculation of steady-state quantities (e.g. ODP). Including a loss term in the calculation, we develop a new formulation of FRF and find that the time dependence can almost be compensated.
Alexandra-Jane Henrot, Tanja Stanelle, Sabine Schröder, Colombe Siegenthaler, Domenico Taraborrelli, and Martin G. Schultz
Geosci. Model Dev., 10, 903–926, https://doi.org/10.5194/gmd-10-903-2017, https://doi.org/10.5194/gmd-10-903-2017, 2017
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This paper describes the basic results of the biogenic emission scheme, based on MEGAN, integrated into the ECHAM6-HAMMOZ chemistry climate model. Sensitivity to vegetation and climate-dependent parameters is also analysed. This version of the model is now suitable for many tropospheric investigations concerning the impact of biogenic volatile organic compound emissions on the ozone budget, secondary aerosol formation, and atmospheric chemistry.
Olaf Morgenstern, Michaela I. Hegglin, Eugene Rozanov, Fiona M. O'Connor, N. Luke Abraham, Hideharu Akiyoshi, Alexander T. Archibald, Slimane Bekki, Neal Butchart, Martyn P. Chipperfield, Makoto Deushi, Sandip S. Dhomse, Rolando R. Garcia, Steven C. Hardiman, Larry W. Horowitz, Patrick Jöckel, Beatrice Josse, Douglas Kinnison, Meiyun Lin, Eva Mancini, Michael E. Manyin, Marion Marchand, Virginie Marécal, Martine Michou, Luke D. Oman, Giovanni Pitari, David A. Plummer, Laura E. Revell, David Saint-Martin, Robyn Schofield, Andrea Stenke, Kane Stone, Kengo Sudo, Taichu Y. Tanaka, Simone Tilmes, Yousuke Yamashita, Kohei Yoshida, and Guang Zeng
Geosci. Model Dev., 10, 639–671, https://doi.org/10.5194/gmd-10-639-2017, https://doi.org/10.5194/gmd-10-639-2017, 2017
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We present a review of the make-up of 20 models participating in the Chemistry–Climate Model Initiative (CCMI). In comparison to earlier such activities, most of these models comprise a whole-atmosphere chemistry, and several of them include an interactive ocean module. This makes them suitable for studying the interactions of tropospheric air quality, stratospheric ozone, and climate. The paper lays the foundation for other studies using the CCMI simulations for scientific analysis.
Sinikka T. Lennartz, Christa A. Marandino, Marc von Hobe, Pau Cortes, Birgit Quack, Rafel Simo, Dennis Booge, Andrea Pozzer, Tobias Steinhoff, Damian L. Arevalo-Martinez, Corinna Kloss, Astrid Bracher, Rüdiger Röttgers, Elliot Atlas, and Kirstin Krüger
Atmos. Chem. Phys., 17, 385–402, https://doi.org/10.5194/acp-17-385-2017, https://doi.org/10.5194/acp-17-385-2017, 2017
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We present new sea surface and marine boundary layer measurements of carbonyl sulfide, the most abundant sulfur gas in the atmosphere, and calculate an oceanic emission estimate. Our results imply that oceanic emissions are very unlikely to account for the missing source in the atmospheric budget that is currently discussed for OCS.
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.
Sara Bacer, Theodoros Christoudias, and Andrea Pozzer
Atmos. Chem. Phys., 16, 15581–15592, https://doi.org/10.5194/acp-16-15581-2016, https://doi.org/10.5194/acp-16-15581-2016, 2016
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We investigate the influence of the North Atlantic Oscillation on atmospheric pollutant transport in the 21st century under a global climate-change scenario, using a coupled atmosphere–chemistry–ocean general circulation model. We find that, at the end of the century, the south-western Mediterranean and northern Africa will see higher pollutant concentrations during positive NAO phases with respect to the past, while a wider part of north Europe will see lower pollutant concentrations.
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.
Duy Cai, Martin Dameris, Hella Garny, Felix Bunzel, Patrick Jöckel, and Phoebe Graf
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2016-870, https://doi.org/10.5194/acp-2016-870, 2016
Revised manuscript not accepted
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Reliable information on weather and climate are of increasing interest for economy, politics and society.
In particular decadal timescales become more and more important. This study focuses on stratospheric processes relevant for the dynamical variability on intra decadal timescale. We apply a so called power spectra analysis. With this method and further analyses we could determine a minimum vertical resolution for numerical models, which is required to capture these processes.
Kathleen A. Mar, Narendra Ojha, Andrea Pozzer, and Tim M. Butler
Geosci. Model Dev., 9, 3699–3728, https://doi.org/10.5194/gmd-9-3699-2016, https://doi.org/10.5194/gmd-9-3699-2016, 2016
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Ground-level ozone is an air pollutant with adverse effects on human and ecosystem health and is also a climate forcer with a significant warming effect. This paper presents the setup and evaluation of a model for ozone air quality over Europe. Within the model evaluation, we compare the use of two commonly used photochemical schemes, and we conclude that uncertainties in the representation of chemistry are important to consider when using air quality models for policy applications.
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.
Bastian Kern and Patrick Jöckel
Geosci. Model Dev., 9, 3639–3654, https://doi.org/10.5194/gmd-9-3639-2016, https://doi.org/10.5194/gmd-9-3639-2016, 2016
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Input and output of large data limit the performance of numerical models on supercomputers. We present an interface for the calculation of online diagnostics in a weather and climate model. These diagnostics are calculated online during the simulation instead of as subsequent post-processing. Depending on the diagnostic, we can reduce the amount of model output.
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.
Mariano Mertens, Astrid Kerkweg, Patrick Jöckel, Holger Tost, and Christiane Hofmann
Geosci. Model Dev., 9, 3545–3567, https://doi.org/10.5194/gmd-9-3545-2016, https://doi.org/10.5194/gmd-9-3545-2016, 2016
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This fourth part in a series of publications describing the newly developed regional chemistry–climate system MECO(n) is dedicated to the evaluation of MECO(n) with respect to tropospheric gas-phase chemistry. For this, a simulation incorporating two regional instances, one over Europe with 50 km resolution and one over Germany with 12 km resolution, is conducted. The model results are compared with satellite, ground-based and aircraft in situ observations.
Hiroshi Yamashita, Volker Grewe, Patrick Jöckel, Florian Linke, Martin Schaefer, and Daisuke Sasaki
Geosci. Model Dev., 9, 3363–3392, https://doi.org/10.5194/gmd-9-3363-2016, https://doi.org/10.5194/gmd-9-3363-2016, 2016
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This study introduces AirTraf v1.0 for climate impact evaluations, which performs global air traffic simulations in the ECHAM5/MESSy Atmospheric Chemistry model. AirTraf simulations were demonstrated with great circle and flight time routing options for a specific winter day, assuming an Airbus A330 aircraft. The results confirmed that AirTraf simulates the air traffic properly for the two options. Calculated flight time, fuel consumption and NOx emission index are comparable to reference data.
Narendra Singh, Raman Solanki, Narendra Ojha, Ruud H. H. Janssen, Andrea Pozzer, and Surendra K. Dhaka
Atmos. Chem. Phys., 16, 10559–10572, https://doi.org/10.5194/acp-16-10559-2016, https://doi.org/10.5194/acp-16-10559-2016, 2016
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Our study presents measurements and model simulations of boundary layer evolution over a mountain peak in the central Himalayas. The observations were made as a part of the Ganges Valley Aerosol Experiment. The implications of biases in model simulated boundary layer towards simulations of trace species is investigated.
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.
Sabine Brinkop, Martin Dameris, Patrick Jöckel, Hella Garny, Stefan Lossow, and Gabriele Stiller
Atmos. Chem. Phys., 16, 8125–8140, https://doi.org/10.5194/acp-16-8125-2016, https://doi.org/10.5194/acp-16-8125-2016, 2016
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This study investigates the water vapour decline in the stratosphere beginning in the year 2000 and other similarly strong stratospheric water vapour reductions. The driving forces are tropical sea surface temperature (SST) changes due to coincidence with a preceding ENSO event and supported by the west to east change of the QBO.
There are indications that both SSTs and the specific dynamical state of the atmosphere contribute to the long period of low water vapour values from 2001 to 2006.
Steffen Beirle, Christoph Hörmann, Patrick Jöckel, Song Liu, Marloes Penning de Vries, Andrea Pozzer, Holger Sihler, Pieter Valks, and Thomas Wagner
Atmos. Meas. Tech., 9, 2753–2779, https://doi.org/10.5194/amt-9-2753-2016, https://doi.org/10.5194/amt-9-2753-2016, 2016
Simone Dietmüller, Patrick Jöckel, Holger Tost, Markus Kunze, Catrin Gellhorn, Sabine Brinkop, Christine Frömming, Michael Ponater, Benedikt Steil, Axel Lauer, and Johannes Hendricks
Geosci. Model Dev., 9, 2209–2222, https://doi.org/10.5194/gmd-9-2209-2016, https://doi.org/10.5194/gmd-9-2209-2016, 2016
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Four new radiation related submodels (RAD, AEROPT, CLOUDOPT, and ORBIT) are available within the MESSy framework now. They are largely based on the original radiation scheme of ECHAM5. RAD simulates radiative transfer, AEROPT calculates aerosol optical properties, CLOUDOPT calculates cloud optical properties, and ORBIT is responsible for Earth orbit calculations. Multiple diagnostic calls of the radiation routine are possible, so radiative forcing can be calculated during the model simulation.
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).
David Cabrera-Perez, Domenico Taraborrelli, Rolf Sander, and Andrea Pozzer
Atmos. Chem. Phys., 16, 6931–6947, https://doi.org/10.5194/acp-16-6931-2016, https://doi.org/10.5194/acp-16-6931-2016, 2016
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The global atmospheric budget and distribution of monocyclic aromatic compounds is estimated, using an atmospheric chemistry general circulation model. Simulation results are evaluated with observations with the goal of understanding emission, production and removal of these compounds. Anthropogenic and biomass burning are the main sources of aromatic compounds to the atmosphere. The main sink is photochemical decomposition and in lesser importance dry deposition.
Michael Löffler, Sabine Brinkop, and Patrick Jöckel
Atmos. Chem. Phys., 16, 6547–6562, https://doi.org/10.5194/acp-16-6547-2016, https://doi.org/10.5194/acp-16-6547-2016, 2016
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After the two major volcanic eruptions of El Chichón in Mexico in 1982 and Mount Pinatubo on the Philippines in 1991, stratospheric water vapour is significantly increased. This results from increased stratospheric heating rates due to volcanic aerosol and the subsequent changes in stratospheric and tropopause temperatures in the tropics. The tropical vertical advection and the South Asian summer monsoon are identified as important sources for the additional water vapour in the stratosphere.
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.
Patrick Jöckel, Holger Tost, Andrea Pozzer, Markus Kunze, Oliver Kirner, Carl A. M. Brenninkmeijer, Sabine Brinkop, Duy S. Cai, Christoph Dyroff, Johannes Eckstein, Franziska Frank, Hella Garny, Klaus-Dirk Gottschaldt, Phoebe Graf, Volker Grewe, Astrid Kerkweg, Bastian Kern, Sigrun Matthes, Mariano Mertens, Stefanie Meul, Marco Neumaier, Matthias Nützel, Sophie Oberländer-Hayn, Roland Ruhnke, Theresa Runde, Rolf Sander, Dieter Scharffe, and Andreas Zahn
Geosci. Model Dev., 9, 1153–1200, https://doi.org/10.5194/gmd-9-1153-2016, https://doi.org/10.5194/gmd-9-1153-2016, 2016
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With an advanced numerical global chemistry climate model (CCM) we performed several detailed
combined hind-cast and projection simulations of the period 1950 to 2100 to assess the
past, present, and potential future dynamical and chemical state of the Earth atmosphere.
The manuscript documents the model and the various applied model set-ups and provides
a first evaluation of the simulation results from a global perspective as a quality check of the data.
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.
A. J. G. Baumgaertner, P. Jöckel, A. Kerkweg, R. Sander, and H. Tost
Geosci. Model Dev., 9, 125–135, https://doi.org/10.5194/gmd-9-125-2016, https://doi.org/10.5194/gmd-9-125-2016, 2016
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The Community Earth System Model (CESM1) is connected to the the Modular Earth Submodel System (MESSy) as a new base model. This allows MESSy users the option to utilize either the state-of-the art spectral element atmosphere dynamical core or the finite volume core of CESM1. Additionally, this makes several other component models available to MESSy users.
Christiane Hofmann, Astrid Kerkweg, Peter Hoor, and Patrick Jöckel
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2015-949, https://doi.org/10.5194/acp-2015-949, 2016
Revised manuscript not accepted
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Ozone enhancements at the surface, caused by descending stratospheric air masses along deep tropopause folds, can be reproduced using the model system MECO(n). It is shown that stratosphere-troposphere-exchange (STE) in the vicinity of a tropopause fold occurs in regions of turbulence and diabatic processes. The efficiency of mixing is quantified, showing that almost all of the air masses originating in the tropopause fold are transported into the troposphere during the following two days.
S. Bacer, T. Christoudias, and A. Pozzer
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-15-33049-2015, https://doi.org/10.5194/acpd-15-33049-2015, 2015
Preprint withdrawn
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We investigate the temporal variability of the North Atlantic Oscillation (NAO) pattern and its relation to the atmospheric dispersion of pollutants in the near past and in the future.
We use a global climate circulation model in order to analyze the NAO signal and its correlation with pollutant concentrations. We find that the NAO is influenced by natural climate variability and that the NAO Indices may be used as indicators of (future) pollutant transport over Europe.
A. Kerkweg and P. Jöckel
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmdd-8-8607-2015, https://doi.org/10.5194/gmdd-8-8607-2015, 2015
Revised manuscript not accepted
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
R. Eichinger, P. Jöckel, and S. Lossow
Atmos. Chem. Phys., 15, 7003–7015, https://doi.org/10.5194/acp-15-7003-2015, https://doi.org/10.5194/acp-15-7003-2015, 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.
R. Eichinger, P. Jöckel, S. Brinkop, M. Werner, and S. Lossow
Atmos. Chem. Phys., 15, 5537–5555, https://doi.org/10.5194/acp-15-5537-2015, https://doi.org/10.5194/acp-15-5537-2015, 2015
A. Pozzer, A. de Meij, J. Yoon, H. Tost, A. K. Georgoulias, and M. Astitha
Atmos. Chem. Phys., 15, 5521–5535, https://doi.org/10.5194/acp-15-5521-2015, https://doi.org/10.5194/acp-15-5521-2015, 2015
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Thanks to numerical simulations and satellite observations, it is shown that aerosol optical depth (AOD) trends (2000--2010 period) over the US and Europe are due to emission decrease, while over the Sahara Desert and the Middle East they are due to meteorological changes. Over Southeast Asia, both meteorology and emission changes are important for the AOD trends.
It is shown that soluble components strongly influence AOD, as their contribution is enhanced by the aerosol water content.
M. Righi, V. Eyring, K.-D. Gottschaldt, C. Klinger, F. Frank, P. Jöckel, and I. Cionni
Geosci. Model Dev., 8, 733–768, https://doi.org/10.5194/gmd-8-733-2015, https://doi.org/10.5194/gmd-8-733-2015, 2015
R. H. H. Janssen and A. Pozzer
Geosci. Model Dev., 8, 453–471, https://doi.org/10.5194/gmd-8-453-2015, https://doi.org/10.5194/gmd-8-453-2015, 2015
R. Oswald, M. Ermel, K. Hens, A. Novelli, H. G. Ouwersloot, P. Paasonen, T. Petäjä, M. Sipilä, P. Keronen, J. Bäck, R. Königstedt, Z. Hosaynali Beygi, H. Fischer, B. Bohn, D. Kubistin, H. Harder, M. Martinez, J. Williams, T. Hoffmann, I. Trebs, and M. Sörgel
Atmos. Chem. Phys., 15, 799–813, https://doi.org/10.5194/acp-15-799-2015, https://doi.org/10.5194/acp-15-799-2015, 2015
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Nitrous acid (HONO) is a key species in atmospheric photochemistry since the photolysis leads to the important hydroxyl radical (OH). Although the importance of HONO as a precursor of OH is known, the formation pathways of HONO, especially during daytime, are a major challenge in atmospheric science. We present a detailed analysis of sources and sinks for HONO in the atmosphere for a field measurement campaign in the boreal forest in Finland and wonder if there is really a source term missing.
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.
R. Sander, P. Jöckel, O. Kirner, A. T. Kunert, J. Landgraf, and A. Pozzer
Geosci. Model Dev., 7, 2653–2662, https://doi.org/10.5194/gmd-7-2653-2014, https://doi.org/10.5194/gmd-7-2653-2014, 2014
C. M. Hoppe, L. Hoffmann, P. Konopka, J.-U. Grooß, F. Ploeger, G. Günther, P. Jöckel, and R. Müller
Geosci. Model Dev., 7, 2639–2651, https://doi.org/10.5194/gmd-7-2639-2014, https://doi.org/10.5194/gmd-7-2639-2014, 2014
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
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
J. Yoon and A. Pozzer
Atmos. Chem. Phys., 14, 10465–10482, https://doi.org/10.5194/acp-14-10465-2014, https://doi.org/10.5194/acp-14-10465-2014, 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. Valks, N. Hao, S. Gimeno Garcia, D. Loyola, M. Dameris, P. Jöckel, and A. Delcloo
Atmos. Meas. Tech., 7, 2513–2530, https://doi.org/10.5194/amt-7-2513-2014, https://doi.org/10.5194/amt-7-2513-2014, 2014
R. Eichinger and P. Jöckel
Geosci. Model Dev., 7, 1573–1582, https://doi.org/10.5194/gmd-7-1573-2014, https://doi.org/10.5194/gmd-7-1573-2014, 2014
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
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
S. Meul, U. Langematz, S. Oberländer, H. Garny, and P. Jöckel
Atmos. Chem. Phys., 14, 2959–2971, https://doi.org/10.5194/acp-14-2959-2014, https://doi.org/10.5194/acp-14-2959-2014, 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
V. Grewe, C. Frömming, S. Matthes, S. Brinkop, M. Ponater, S. Dietmüller, P. Jöckel, H. Garny, E. Tsati, K. Dahlmann, O. A. Søvde, J. Fuglestvedt, T. K. Berntsen, K. P. Shine, E. A. Irvine, T. Champougny, and P. Hullah
Geosci. Model Dev., 7, 175–201, https://doi.org/10.5194/gmd-7-175-2014, https://doi.org/10.5194/gmd-7-175-2014, 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
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
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
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
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
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
K. Gottschaldt, C. Voigt, P. Jöckel, M. Righi, R. Deckert, and S. Dietmüller
Atmos. Chem. Phys., 13, 3003–3025, https://doi.org/10.5194/acp-13-3003-2013, https://doi.org/10.5194/acp-13-3003-2013, 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
Related subject area
Subject: Gases | Research Activity: Field Measurements | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Shipping and algae emissions have a major impact on ambient air mixing ratios of non-methane hydrocarbons (NMHCs) and methanethiol on Utö Island in the Baltic Sea
Contribution of cooking emissions to the urban volatile organic compounds in Las Vegas, NV
Reanalysis of NOAA H2 observations: implications for the H2 budget
A large role of missing volatile organic compound reactivity from anthropogenic emissions in ozone pollution regulation
Measurement report: Insights into the chemical composition and origin of molecular clusters and potential precursor molecules present in the free troposphere over the southern Indian Ocean: observations from the Maïdo Observatory (2150 m a.s.l., Réunion)
Production of oxygenated volatile organic compounds from the ozonolysis of coastal seawater
Comment on “Transport of substantial stratospheric ozone to the surface by a dying typhoon and shallow convection” by Chen et al. (2022)
Observations of cyanogen bromide (BrCN) in the global troposphere and their relation to polar surface O3 destruction
Individual coal mine methane emissions constrained by eddy covariance measurements: low bias and missing sources
Measurement report: Observations of ground-level ozone concentration gradients perpendicular to the Lake Ontario shoreline
Measurement report: The Palau Atmospheric Observatory and its ozonesonde record – continuous monitoring of tropospheric composition and dynamics in the tropical western Pacific
Quantifying SO2 oxidation pathways to atmospheric sulfate using stable sulfur and oxygen isotopes: laboratory simulation and field observation
Influences of downward transport and photochemistry on surface ozone over East Antarctica during austral summer: in situ observations and model simulations
Iodine oxoacids and their roles in sub-3 nm particle growth in polluted urban environments
Intensive photochemical oxidation in the marine atmosphere: evidence from direct radical measurements
Diurnal variations in oxygen and nitrogen isotopes of atmospheric nitrogen dioxide and nitrate: implications for tracing NOx oxidation pathways and emission sources
Measurement report: Method for evaluating CO2 emissions from a cement plant using atmospheric δ(O2 ∕ N2) and CO2 measurements and its implication for future detection of CO2 capture signals
Aircraft-based mass balance estimate of methane emissions from offshore gas facilities in the southern North Sea
Parameterizations of US wildfire and prescribed fire emission ratios and emission factors based on FIREX-AQ aircraft measurements
Measurement report: Atmospheric nitrate radical chemistry in the South China Sea influenced by the urban outflow of the Pearl River Delta
The interhemispheric gradient of SF6 in the upper troposphere
Weather regimes and the related atmospheric composition at a Pyrenean observatory characterized by hierarchical clustering of a 5-year data set
Tropospheric bromine monoxide vertical profiles retrieved across the Alaskan Arctic in springtime
Source apportionment of methane emissions from the Upper Silesian Coal Basin using isotopic signatures
Measurement report: Exchange fluxes of HONO over agricultural fields in the North China Plain
HONO chemistry at a suburban site during the EXPLORE-YRD campaign in 2018: formation mechanisms and impacts on O3 production
Evaluation of modelled climatologies of O3, CO, water vapour and NOy in the upper troposphere–lower stratosphere using regular in situ observations by passenger aircraft
Photochemical ageing of aerosols contributes significantly to the production of atmospheric formic acid
Nitrous acid budgets in the coastal atmosphere: potential daytime marine sources
Sources of organic gases and aerosol particles and their roles in nighttime particle growth at a rural forested site in southwest Germany
Undetected biogenic volatile organic compounds from Norway spruce drive total ozone reactivity measurements
Quantification of fossil fuel CO2 from combined CO, δ13CO2 and Δ14CO2 observations
Radical chemistry and ozone production at a UK coastal receptor site
Sources and long-term variability of carbon monoxide at Mount Kenya and in Nairobi
Opinion: Strengthening Research in the Global South: Atmospheric Science Opportunities in South America and Africa
Measurement report: Airborne measurements of NOx fluxes over Los Angeles during the RECAP-CA 2021 campaign
Influence of anthropogenic emissions on the composition of highly oxygenated organic molecules in Helsinki: a street canyon and urban background station comparison
Changes in surface ozone in South Korea on diurnal to decadal timescales for the period of 2001–2021
Characterization of the nitrogen stable isotope composition (δ15N) of ship-emitted NOx
Volatile organic compound fluxes in the agricultural San Joaquin Valley – spatial distribution, source attribution, and inventory comparison
Exploring the amplified role of HCHO in the formation of HMS and O3 during the co-occurring PM2.5 and O3 pollution in a coastal city of southeast China
High potential for CH4 emission mitigation from oil infrastructure in one of EU's major production regions
Measurement report: Source apportionment and environmental impacts of volatile organic compounds (VOCs) in Lhasa, a highland city in China
OH, HO2, and RO2 radical chemistry in a rural forest environment: measurements, model comparisons, and evidence of a missing radical sink
The atmospheric fate of 1,2-dibromo-4-(1,2-dibromoethyl)cyclohexane (TBECH): spatial patterns, seasonal variability, and deposition to Canadian coastal regions
A single-point modeling approach for the intercomparison and evaluation of ozone dry deposition across chemical transport models (Activity 2 of AQMEII4)
Direct observations of NOx emissions over the San Joaquin Valley using airborne flux measurements during RECAP-CA 2021 field campaign
Surface snow bromide and nitrate at Eureka, Canada in early spring and implications for polar boundary layer chemistry
Trends and seasonal variability in ammonia across major biomes in western and central Africa inferred from long-term series of ground-based and satellite measurements
A rise in HFC-23 emissions from eastern Asia since 2015
Heidi Hellén, Rostislav Kouznetsov, Kaisa Kraft, Jukka Seppälä, Mika Vestenius, Jukka-Pekka Jalkanen, Lauri Laakso, and Hannele Hakola
Atmos. Chem. Phys., 24, 4717–4731, https://doi.org/10.5194/acp-24-4717-2024, https://doi.org/10.5194/acp-24-4717-2024, 2024
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Mixing ratios of C2-C5 NMHCs and methanethiol were measured on an island in the Baltic Sea using an in situ gas chromatograph. Shipping emissions were found to be an important source of ethene, ethyne, propene, and benzene. High summertime mixing ratios of methanethiol and dependence of mixing ratios on seawater temperature and height indicated the biogenic origin to possibly be phytoplankton or macroalgae. These emissions may have a strong impact on SO2 production and new particle formation.
Matthew M. Coggon, Chelsea E. Stockwell, Lu Xu, Jeff Peischl, Jessica B. Gilman, Aaron Lamplugh, Henry J. Bowman, Kenneth Aikin, Colin Harkins, Qindan Zhu, Rebecca H. Schwantes, Jian He, Meng Li, Karl Seltzer, Brian McDonald, and Carsten Warneke
Atmos. Chem. Phys., 24, 4289–4304, https://doi.org/10.5194/acp-24-4289-2024, https://doi.org/10.5194/acp-24-4289-2024, 2024
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Residential and commercial cooking emits pollutants that degrade air quality. Here, ambient observations show that cooking is an important contributor to anthropogenic volatile organic compounds (VOCs) emitted in Las Vegas, NV. These emissions are not fully presented in air quality models, and more work may be needed to quantify emissions from important sources, such as commercial restaurants.
Fabien Paulot, Gabrielle Pétron, Andrew M. Crotwell, and Matteo B. Bertagni
Atmos. Chem. Phys., 24, 4217–4229, https://doi.org/10.5194/acp-24-4217-2024, https://doi.org/10.5194/acp-24-4217-2024, 2024
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New data from the National Oceanic and Atmospheric Administration show that hydrogen (H2) concentrations increased from 2010 to 2019, which is consistent with the simulated increase in H2 photochemical production (mainly from methane). But this cannot be reconciled with the expected decrease (increase) in H2 anthropogenic emissions (soil deposition) in the same period. This shows gaps in our knowledge of the H2 biogeochemical cycle that must be resolved to quantify the impact of higher H2 usage.
Wenjie Wang, Bin Yuan, Hang Su, Yafang Cheng, Jipeng Qi, Sihang Wang, Wei Song, Xinming Wang, Chaoyang Xue, Chaoqun Ma, Fengxia Bao, Hongli Wang, Shengrong Lou, and Min Shao
Atmos. Chem. Phys., 24, 4017–4027, https://doi.org/10.5194/acp-24-4017-2024, https://doi.org/10.5194/acp-24-4017-2024, 2024
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This study investigates the important role of unmeasured volatile organic compounds (VOCs) in ozone formation. Based on results in a megacity of China, we show that unmeasured VOCs can contribute significantly to ozone fomation and also influence the determination of ozone control strategy. Our results show that these unmeasured VOCs are mainly from human sources.
Romain Salignat, Matti Rissanen, Siddharth Iyer, Jean-Luc Baray, Pierre Tulet, Jean-Marc Metzger, Jérôme Brioude, Karine Sellegri, and Clémence Rose
Atmos. Chem. Phys., 24, 3785–3812, https://doi.org/10.5194/acp-24-3785-2024, https://doi.org/10.5194/acp-24-3785-2024, 2024
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Using mass spectrometry data collected at the Maïdo Observatory (2160 m a.s.l., Réunion), we provide the first detailed analysis of molecular cluster chemical composition specifically in the marine free troposphere. The abundance of the identified species is related both to in situ meteorological parameters and air mass history, which also provide insight into their origin. Our work makes an important contribution to documenting the chemistry and physics of the marine free troposphere.
Delaney B. Kilgour, Gordon A. Novak, Megan S. Claflin, Brian M. Lerner, and Timothy H. Bertram
Atmos. Chem. Phys., 24, 3729–3742, https://doi.org/10.5194/acp-24-3729-2024, https://doi.org/10.5194/acp-24-3729-2024, 2024
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Laboratory experiments with seawater mimics suggest ozone deposition to the surface ocean can be a source of reactive carbon to the marine atmosphere. We conduct both field and laboratory measurements to assess abiotic VOC composition and yields from ozonolysis of real surface seawater. We show that C5–C11 aldehydes contribute to the observed VOC emission flux. We estimate that VOCs generated by the ozonolysis of surface seawater are competitive with biological VOC production and emission.
Xiangdong Zheng, Wen Yang, Yuting Sun, Chunmei Geng, Yingying Liu, and Xiaobin Xu
Atmos. Chem. Phys., 24, 3759–3768, https://doi.org/10.5194/acp-24-3759-2024, https://doi.org/10.5194/acp-24-3759-2024, 2024
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Chen et al. (2022) attributed the nocturnal ozone enhancement (NOE) during the night of 31 July 2021 in the North China Plain (NCP) to "the direct stratospheric intrusion to reach the surface". We analyzed in situ data from the NCP. Our results do not suggest that there was a significant impact from the stratosphere on surface ozone during the NOE. We argue that the NOE was not caused by stratospheric intrusion but originated from fresh photochemical production in the lower troposphere.
James M. Roberts, Siyuan Wang, Patrick R. Veres, J. Andrew Neuman, Michael A. Robinson, Ilann Bourgeois, Jeff Peischl, Thomas B. Ryerson, Chelsea R. Thompson, Hannah M. Allen, John D. Crounse, Paul O. Wennberg, Samuel R. Hall, Kirk Ullmann, Simone Meinardi, Isobel J. Simpson, and Donald Blake
Atmos. Chem. Phys., 24, 3421–3443, https://doi.org/10.5194/acp-24-3421-2024, https://doi.org/10.5194/acp-24-3421-2024, 2024
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We measured cyanogen bromide (BrCN) in the troposphere for the first time. BrCN is a product of the same active bromine chemistry that destroys ozone and removes mercury in polar surface environments and is a previously unrecognized sink for active Br compounds. BrCN has an apparent lifetime against heterogeneous loss in the range 1–10 d, so it serves as a cumulative marker of Br-radical chemistry. Accounting for BrCN chemistry is an important part of understanding polar Br cycling.
Kai Qin, Wei Hu, Qin He, Fan Lu, and Jason Blake Cohen
Atmos. Chem. Phys., 24, 3009–3028, https://doi.org/10.5194/acp-24-3009-2024, https://doi.org/10.5194/acp-24-3009-2024, 2024
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We compute CH4 emissions and uncertainty on a mine-by-mine basis, including underground, overground, and abandoned mines. Mine-by-mine gas and flux data and 30 min observations from a flux tower located next to a mine shaft are integrated. The observed variability and bias correction are propagated over the emissions dataset, demonstrating that daily observations may not cover the range of variability. Comparisons show both an emissions magnitude and spatial mismatch with current inventories.
Yao Yan Huang and D. James Donaldson
Atmos. Chem. Phys., 24, 2387–2398, https://doi.org/10.5194/acp-24-2387-2024, https://doi.org/10.5194/acp-24-2387-2024, 2024
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Ground-level ozone interacts at the lake–land boundary; this is important to our understanding and modelling of atmospheric chemistry and air pollution in the lower atmosphere. We show that a steep ozone gradient occurs year-round moving inland up to 1 km from the lake and that this gradient is influenced by seasonal factors on the local land environment, where more rural areas are more greatly affected seasonally.
Katrin Müller, Jordis S. Tradowsky, Peter von der Gathen, Christoph Ritter, Sharon Patris, Justus Notholt, and Markus Rex
Atmos. Chem. Phys., 24, 2169–2193, https://doi.org/10.5194/acp-24-2169-2024, https://doi.org/10.5194/acp-24-2169-2024, 2024
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The Palau Atmospheric Observatory is introduced as an ideal site to detect changes in atmospheric composition and dynamics above the remote tropical western Pacific. We focus on the ozone sounding program from 2016–2021, including El Niño 2016. The year-round high convective activity is reflected in dominant low tropospheric ozone and high relative humidity. Their seasonal distributions are unique compared to other tropical sites and are modulated by the Intertropical Convergence Zone.
Ziyan Guo, Keding Lu, Pengxiang Qiu, Mingyi Xu, and Zhaobing Guo
Atmos. Chem. Phys., 24, 2195–2205, https://doi.org/10.5194/acp-24-2195-2024, https://doi.org/10.5194/acp-24-2195-2024, 2024
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The formation of secondary sulfate needs to be further explored. In this work, we simultaneously measured sulfur and oxygen isotopic compositions to gain an increased understanding of specific sulfate formation processes. The results indicated that secondary sulfate was mainly ascribed to SO2 homogeneous oxidation by OH radicals and heterogeneous oxidation by H2O2 and Fe3+ / O2. This study is favourable for deeply investigating the sulfur cycle in the atmosphere.
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.
Ying Zhang, Duzitian Li, Xu-Cheng He, Wei Nie, Chenjuan Deng, Runlong Cai, Yuliang Liu, Yishuo Guo, Chong Liu, Yiran Li, Liangduo Chen, Yuanyuan Li, Chenjie Hua, Tingyu Liu, Zongcheng Wang, Jiali Xie, Lei Wang, Tuukka Petäjä, Federico Bianchi, Ximeng Qi, Xuguang Chi, Pauli Paasonen, Yongchun Liu, Chao Yan, Jingkun Jiang, Aijun Ding, and Markku Kulmala
Atmos. Chem. Phys., 24, 1873–1893, https://doi.org/10.5194/acp-24-1873-2024, https://doi.org/10.5194/acp-24-1873-2024, 2024
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This study conducts a long-term observation of gaseous iodine oxoacids in two Chinese megacities, revealing their ubiquitous presence with peak concentrations (up to 0.1 pptv) in summer. Our analysis suggests a mix of terrestrial and marine sources for iodine. Additionally, iodic acid is identified as a notable contributor to sub-3 nm particle growth and particle survival probability.
Guoxian Zhang, Renzhi Hu, Pinhua Xie, Changjin Hu, Xiaoyan Liu, Liujun Zhong, Haotian Cai, Bo Zhu, Shiyong Xia, Xiaofeng Huang, Xin Li, and Wenqing Liu
Atmos. Chem. Phys., 24, 1825–1839, https://doi.org/10.5194/acp-24-1825-2024, https://doi.org/10.5194/acp-24-1825-2024, 2024
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Comprehensive observation of HOx radicals was conducted at a coastal site in the Pearl River Delta. Radical chemistry was influenced by different air masses in a time-dependent way. Land mass promotes a more active photochemical process, with daily averages of 7.1 × 106 and 5.2 × 108 cm−3 for OH and HO2 respectively. The rapid oxidation process was accompanied by a higher diurnal HONO concentration, which influences the ozone-sensitive system and eventually magnifies the background ozone.
Sarah Albertin, Joël Savarino, Slimane Bekki, Albane Barbero, Roberto Grilli, Quentin Fournier, Irène Ventrillard, Nicolas Caillon, and Kathy Law
Atmos. Chem. Phys., 24, 1361–1388, https://doi.org/10.5194/acp-24-1361-2024, https://doi.org/10.5194/acp-24-1361-2024, 2024
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This study reports the first simultaneous records of oxygen (Δ17O) and nitrogen (δ15N) isotopes in nitrogen dioxide (NO2) and nitrate (NO3−). These data are combined with atmospheric observations to explore sub-daily N reactive chemistry and quantify N fractionation effects in an Alpine winter city. The results highlight the necessity of using Δ17O and δ15N in both NO2 and NO3− to avoid biased estimations of NOx sources and fates from NO3− isotopic records in urban winter environments.
Shigeyuki Ishidoya, Kazuhiro Tsuboi, Hiroaki Kondo, Kentaro Ishijima, Nobuyuki Aoki, Hidekazu Matsueda, and Kazuyuki Saito
Atmos. Chem. Phys., 24, 1059–1077, https://doi.org/10.5194/acp-24-1059-2024, https://doi.org/10.5194/acp-24-1059-2024, 2024
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A method evaluating techniques for carbon neutrality, such as carbon capture and storage (CCS), is important. This study presents a method to evaluate CO2 emissions from a cement plant based on atmospheric O2 and CO2 measurements. The method will also be useful for evaluating CO2 capture from flue gas at CCS plants, since the plants remove CO2 from the atmosphere without causing any O2 changes, just as cement plants do, differing only in the direction of CO2 exchange with the atmosphere.
Magdalena Pühl, Anke Roiger, Alina Fiehn, Alan M. Gorchov Negron, Eric A. Kort, Stefan Schwietzke, Ignacio Pisso, Amy Foulds, James Lee, James L. France, Anna E. Jones, Dave Lowry, Rebecca E. Fisher, Langwen Huang, Jacob Shaw, Prudence Bateson, Stephen Andrews, Stuart Young, Pamela Dominutti, Tom Lachlan-Cope, Alexandra Weiss, and Grant Allen
Atmos. Chem. Phys., 24, 1005–1024, https://doi.org/10.5194/acp-24-1005-2024, https://doi.org/10.5194/acp-24-1005-2024, 2024
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In April–May 2019 we carried out an airborne field campaign in the southern North Sea with the aim of studying methane emissions of offshore gas installations. We determined methane emissions from elevated methane measured downstream of the sampled installations. We compare our measured methane emissions with estimated methane emissions from national and global annual inventories. As a result, we find inconsistencies of inventories and large discrepancies between measurements and inventories.
Georgios I. Gkatzelis, Matthew M. Coggon, Chelsea E. Stockwell, Rebecca S. Hornbrook, Hannah Allen, Eric C. Apel, Megan M. Bela, Donald R. Blake, Ilann Bourgeois, Steven S. Brown, Pedro Campuzano-Jost, Jason M. St. Clair, James H. Crawford, John D. Crounse, Douglas A. Day, Joshua P. DiGangi, Glenn S. Diskin, Alan Fried, Jessica B. Gilman, Hongyu Guo, Johnathan W. Hair, Hannah S. Halliday, Thomas F. Hanisco, Reem Hannun, Alan Hills, L. Gregory Huey, Jose L. Jimenez, Joseph M. Katich, Aaron Lamplugh, Young Ro Lee, Jin Liao, Jakob Lindaas, Stuart A. McKeen, Tomas Mikoviny, Benjamin A. Nault, J. Andrew Neuman, John B. Nowak, Demetrios Pagonis, Jeff Peischl, Anne E. Perring, Felix Piel, Pamela S. Rickly, Michael A. Robinson, Andrew W. Rollins, Thomas B. Ryerson, Melinda K. Schueneman, Rebecca H. Schwantes, Joshua P. Schwarz, Kanako Sekimoto, Vanessa Selimovic, Taylor Shingler, David J. Tanner, Laura Tomsche, Krystal T. Vasquez, Patrick R. Veres, Rebecca Washenfelder, Petter Weibring, Paul O. Wennberg, Armin Wisthaler, Glenn M. Wolfe, Caroline C. Womack, Lu Xu, Katherine Ball, Robert J. Yokelson, and Carsten Warneke
Atmos. Chem. Phys., 24, 929–956, https://doi.org/10.5194/acp-24-929-2024, https://doi.org/10.5194/acp-24-929-2024, 2024
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This study reports emissions of gases and particles from wildfires. These emissions are related to chemical proxies that can be measured by satellite and incorporated into models to improve predictions of wildfire impacts on air quality and climate.
Jie Wang, Haichao Wang, Yee Jun Tham, Lili Ming, Zelong Zheng, Guizhen Fang, Cuizhi Sun, Zhenhao Ling, Jun Zhao, and Shaojia Fan
Atmos. Chem. Phys., 24, 977–992, https://doi.org/10.5194/acp-24-977-2024, https://doi.org/10.5194/acp-24-977-2024, 2024
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Many works report NO3 chemistry in inland regions while less target marine regions. We measured N2O5 and related species on a typical island and found intensive nighttime chemistry and rapid NO3 loss. NO contributed significantly to NO3 loss despite its sub-ppbv level, suggesting nocturnal NO3 reactions would be largely enhanced once free from NO emissions in the open ocean. This highlights the strong influences of urban outflow on downward marine areas in terms of nighttime chemistry.
Tanja J. Schuck, Johannes Degen, Eric Hintsa, Peter Hoor, Markus Jesswein, Timo Keber, Daniel Kunkel, Fred Moore, Florian Obersteiner, Matt Rigby, Thomas Wagenhäuser, Luke M. Western, Andreas Zahn, and Andreas Engel
Atmos. Chem. Phys., 24, 689–705, https://doi.org/10.5194/acp-24-689-2024, https://doi.org/10.5194/acp-24-689-2024, 2024
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We study the interhemispheric gradient of sulfur hexafluoride (SF6), a strong long-lived greenhouse gas. Its emissions are stronger in the Northern Hemisphere; therefore, mixing ratios in the Southern Hemisphere lag behind. Comparing the observations to a box model, the model predicts air in the Southern Hemisphere to be older. For a better agreement, the emissions used as model input need to be increased (and their spatial pattern changed), and we need to modify north–south transport.
Jérémy Gueffier, François Gheusi, Marie Lothon, Véronique Pont, Alban Philibert, Fabienne Lohou, Solène Derrien, Yannick Bezombes, Gilles Athier, Yves Meyerfeld, Antoine Vial, and Emmanuel Leclerc
Atmos. Chem. Phys., 24, 287–316, https://doi.org/10.5194/acp-24-287-2024, https://doi.org/10.5194/acp-24-287-2024, 2024
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This study investigates the link between weather regime and atmospheric composition at a Pyrenean observatory. Five years of meteorological data were synchronized on a daily basis and then, using a clustering method, separated into six groups of observation days, with most showing marked characteristics of different weather regimes (fair and disturbed weather, winter windstorms, foehn). Statistical differences in gas and particle concentrations appeared between the groups and are discussed.
Nathaniel Brockway, Peter K. Peterson, Katja Bigge, Kristian D. Hajny, Paul B. Shepson, Kerri A. Pratt, Jose D. Fuentes, Tim Starn, Robert Kaeser, Brian H. Stirm, and William R. Simpson
Atmos. Chem. Phys., 24, 23–40, https://doi.org/10.5194/acp-24-23-2024, https://doi.org/10.5194/acp-24-23-2024, 2024
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Bromine monoxide (BrO) strongly affects atmospheric chemistry in the springtime Arctic, yet there are still many uncertainties around its sources and recycling, particularly in the context of a rapidly changing Arctic. In this study, we observed BrO as a function of altitude above the Alaskan Arctic. We found that BrO was often most concentrated near the ground, confirming the ability of snow to produce and recycle reactive bromine, and identified four common vertical distributions of BrO.
Alina Fiehn, Maximilian Eckl, Julian Kostinek, Michał Gałkowski, Christoph Gerbig, Michael Rothe, Thomas Röckmann, Malika Menoud, Hossein Maazallahi, Martina Schmidt, Piotr Korbeń, Jarosław Neçki, Mila Stanisavljević, Justyna Swolkień, Andreas Fix, and Anke Roiger
Atmos. Chem. Phys., 23, 15749–15765, https://doi.org/10.5194/acp-23-15749-2023, https://doi.org/10.5194/acp-23-15749-2023, 2023
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During the CoMet mission in the Upper Silesian Coal Basin (USCB) ground-based and airborne air samples were taken and analyzed for the isotopic composition of CH4 to derive the mean signature of the USCB and source signatures of individual coal mines. Using δ2H signatures, the biogenic emissions from the USCB account for 15 %–50 % of total emissions, which is underestimated in common emission inventories. This demonstrates the importance of δ2H-CH4 observations for methane source apportionment.
Yifei Song, Chaoyang Xue, Yuanyuan Zhang, Pengfei Liu, Fengxia Bao, Xuran Li, and Yujing Mu
Atmos. Chem. Phys., 23, 15733–15747, https://doi.org/10.5194/acp-23-15733-2023, https://doi.org/10.5194/acp-23-15733-2023, 2023
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We present measurements of HONO flux and related parameters over an agricultural field during a whole growing season of summer maize. This dataset allows studies on the characteristics and influencing factors of soil HONO emissions, determination of HONO emission factors, estimation of total HONO emissions at a national scale, and the discussion on future environmental policies in terms of mitigating regional air pollution.
Can Ye, Keding Lu, Xuefei Ma, Wanyi Qiu, Shule Li, Xinping Yang, Chaoyang Xue, Tianyu Zhai, Yuhan Liu, Xuan Li, Yang Li, Haichao Wang, Zhaofeng Tan, Xiaorui Chen, Huabin Dong, Limin Zeng, Min Hu, and Yuanhang Zhang
Atmos. Chem. Phys., 23, 15455–15472, https://doi.org/10.5194/acp-23-15455-2023, https://doi.org/10.5194/acp-23-15455-2023, 2023
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In this study, combining comprehensive field measurements and a box model, we found NO2 conversion on the ground surface was the most important source for HONO production among the proposed heterogeneous and gas-phase HONO sources. In addition, HONO was found to evidently enhance O3 production and aggravate O3 pollution in summer in China. Our study improved our understanding of the relative importance of different HONO sources and the crucial role of HONO in O3 formation in polluted areas.
Yann Cohen, Didier Hauglustaine, Bastien Sauvage, Susanne Rohs, Patrick Konjari, Ulrich Bundke, Andreas Petzold, Valérie Thouret, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 23, 14973–15009, https://doi.org/10.5194/acp-23-14973-2023, https://doi.org/10.5194/acp-23-14973-2023, 2023
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The upper troposphere–lower stratosphere (UTLS) is a key region regarding the lower atmospheric composition. This study consists of a comprehensive evaluation of an up-to-date chemistry–climate model in this layer, using regular in situ measurements based on passenger aircraft. For this purpose, a specific software (Interpol-IAGOS) has been updated and made publicly available. The model reproduces the carbon monoxide peaks due to biomass burning over the continental tropics particularly well.
Yifan Jiang, Men Xia, Zhe Wang, Penggang Zheng, Yi Chen, and Tao Wang
Atmos. Chem. Phys., 23, 14813–14828, https://doi.org/10.5194/acp-23-14813-2023, https://doi.org/10.5194/acp-23-14813-2023, 2023
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This study provides the first estimate of high rates of formic acid (HCOOH) production from the photochemical aging of real ambient particles and demonstrates the potential importance of this pathway in the formation of HCOOH under ambient conditions. Incorporating this pathway significantly improved the performance of a widely used chemical model. Our solution irradiation experiments demonstrated the importance of nitrate photolysis in HCOOH production via the production of oxidants.
Xuelian Zhong, Hengqing Shen, Min Zhao, Ji Zhang, Yue Sun, Yuhong Liu, Yingnan Zhang, Ye Shan, Hongyong Li, Jiangshan Mu, Yu Yang, Yanqiu Nie, Jinghao Tang, Can Dong, Xinfeng Wang, Yujiao Zhu, Mingzhi Guo, Wenxing Wang, and Likun Xue
Atmos. Chem. Phys., 23, 14761–14778, https://doi.org/10.5194/acp-23-14761-2023, https://doi.org/10.5194/acp-23-14761-2023, 2023
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Nitrous acid (HONO) is vital for atmospheric oxidation. In research at Mount Lao, China, models revealed a significant unidentified marine HONO source. Overlooking this could skew our understanding of air quality and climate change. This finding emphasizes HONO’s importance in the coastal atmosphere, uncovering previously unnoticed interactions.
Junwei Song, Harald Saathoff, Feng Jiang, Linyu Gao, Hengheng Zhang, and Thomas Leisner
EGUsphere, https://doi.org/10.5194/egusphere-2023-2255, https://doi.org/10.5194/egusphere-2023-2255, 2023
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This study presents the concurrent online measurements of organic gas and particles (VOCs and OA) at a forest 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 contribute significantly to nighttime particle growth. The results help to understand the causes of nighttime particle growth regularly observed in summer in the central European rural forested environments.
Steven Job Thomas, Toni Tykkä, Heidi Hellén, Federico Bianchi, and Arnaud P. Praplan
Atmos. Chem. Phys., 23, 14627–14642, https://doi.org/10.5194/acp-23-14627-2023, https://doi.org/10.5194/acp-23-14627-2023, 2023
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The study employed total ozone reactivity to demonstrate how emissions of Norway spruce readily react with ozone and could be a major ozone sink, particularly under stress. Additionally, this approach provided insight into the limitations of current analytical techniques that measure the compounds present or emitted into the atmosphere. The study shows how the technique used was not enough to measure all compounds emitted, and this could potentially underestimate various atmospheric processes.
Jinsol Kim, John B. Miller, Charles E. Miller, Scott J. Lehman, Sylvia E. Michel, Vineet Yadav, Nick E. Rollins, and William M. Berelson
Atmos. Chem. Phys., 23, 14425–14436, https://doi.org/10.5194/acp-23-14425-2023, https://doi.org/10.5194/acp-23-14425-2023, 2023
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In this study, we present the partitioning of CO2 signals from biogenic, petroleum and natural gas sources by combining CO, 13CO2 and 14CO2 measurements. Using measurements from flask air samples at three sites in the greater Los Angeles region, we find larger and positive contributions of biogenic signals in winter and smaller and negative contributions in summer. The largest contribution of natural gas combustion generally occurs in summer.
Robert Woodward-Massey, Roberto Sommariva, Lisa K. Whalley, Danny R. Cryer, Trevor Ingham, William J. Bloss, Stephen M. Ball, Sam Cox, James D. Lee, Chris P. Reed, Leigh R. Crilley, Louisa J. Kramer, Brian J. Bandy, Grant L. Forster, Claire E. Reeves, Paul S. Monks, and Dwayne E. Heard
Atmos. Chem. Phys., 23, 14393–14424, https://doi.org/10.5194/acp-23-14393-2023, https://doi.org/10.5194/acp-23-14393-2023, 2023
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Measurements of OH, HO2 and RO2 radicals and also OH reactivity were made at a UK coastal site and compared to calculations from a constrained box model utilising the Master Chemical Mechanism. The model agreement displayed a strong dependence on the NO concentration. An experimental budget analysis for OH, HO2, RO2 and total ROx demonstrated significant imbalances between HO2 and RO2 production rates. Ozone production rates were calculated from measured radicals and compared to modelled values.
Leonard Kirago, Örjan Gustafsson, Samuel Mwaniki Gaita, Sophie L. Haslett, Michael J. Gatari, Maria Elena Popa, Thomas Röckmann, Christoph Zellweger, Martin Steinbacher, Jörg Klausen, Christian Félix, David Njiru, and August Andersson
Atmos. Chem. Phys., 23, 14349–14357, https://doi.org/10.5194/acp-23-14349-2023, https://doi.org/10.5194/acp-23-14349-2023, 2023
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This study provides ground-observational evidence that supports earlier suggestions that savanna fires are the main emitters and modulators of carbon monoxide gas in Africa. Using isotope-based techniques, the study has shown that about two-thirds of this gas is emitted from savanna fires, while for urban areas, in this case Nairobi, primary sources approach 100 %. The latter has implications for air quality policy, suggesting primary emissions such as traffic should be targeted.
Rebecca M. Garland, Katye E. Altieri, Laura Dawidowski, Laura Gallardo, Aderiana Mbandi, Nestor Y. Rojas, and N'datchoh E. Touré
EGUsphere, https://doi.org/10.5194/egusphere-2023-2566, https://doi.org/10.5194/egusphere-2023-2566, 2023
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In this opinion, we focus on two geographical areas in the Global South to discuss some common challenges and constraints, with a focus on our strengths in atmospheric science research. It is these strengths, we believe, that highlight the critical role of Global South researchers in the future of atmospheric science research.
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.
Magdalena Okuljar, Olga Garmash, Miska Olin, Joni Kalliokoski, Hilkka Timonen, Jarkko V. Niemi, Pauli Paasonen, Jenni Kontkanen, Yanjun Zhang, Heidi Hellén, Heino Kuuluvainen, Minna Aurela, Hanna E. Manninen, Mikko Sipilä, Topi Rönkkö, Tuukka Petäjä, Markku Kulmala, Miikka Dal Maso, and Mikael Ehn
Atmos. Chem. Phys., 23, 12965–12983, https://doi.org/10.5194/acp-23-12965-2023, https://doi.org/10.5194/acp-23-12965-2023, 2023
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Highly oxygenated organic molecules (HOMs) form secondary organic aerosol that affects air quality and health. In this study, we demonstrate that in a moderately polluted city with abundant vegetation, the composition of HOMs is largely controlled by the effect of NOx on the biogenic volatile organic compound oxidation. Comparing the results from two nearby stations, we show that HOM composition and formation pathways can change considerably within small distances in urban environments.
Si-Wan Kim, Kyoung-Min Kim, Yujoo Jeong, Seunghwan Seo, Yeonsu Park, and Jeongyeon Kim
Atmos. Chem. Phys., 23, 12867–12886, https://doi.org/10.5194/acp-23-12867-2023, https://doi.org/10.5194/acp-23-12867-2023, 2023
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Surface ozone is a pollutant regulated for public health. This study derived surface ozone trends over South Korea from 2001 to 2021 and highlighted that South Korea has been a nonattainment area since 2010, based on the US EPA standard. However, the occurrences of high ozone condition decreased in spring during the COVID-19 pandemic, partly due to large reductions of ozone precursor concentrations in China and South Korea.
Zeyu Sun, Zheng Zong, Yang Tan, Chongguo Tian, Zeyu Liu, Fan Zhang, Rong Sun, Yingjun Chen, Jun Li, and Gan Zhang
Atmos. Chem. Phys., 23, 12851–12865, https://doi.org/10.5194/acp-23-12851-2023, https://doi.org/10.5194/acp-23-12851-2023, 2023
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This is the first report of ship-emitted nitrogen stable isotope composition (δ15N) of nitrogen oxides (NOx). The results showed that δ15N–NOx from ships was −18.5 ± 10.9 ‰ and increased monotonically with tightening emission regulations. The selective catalytic reduction system was the most vital factor. The temporal variation in δ15N–NOx was evaluated and can be used to select suitable δ15N–NOx for a more accurate assessment of the contribution of ship-emitted exhaust to atmospheric NOx.
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.
Youwei Hong, Keran Zhang, Dan Liao, Gaojie Chen, Min Zhao, Yiling Lin, Xiaoting Ji, Ke Xu, Yu Wu, Ruilian Yu, Gongren Hu, Sung-Deuk Choi, Likun Xue, and Jinsheng Chen
Atmos. Chem. Phys., 23, 10795–10807, https://doi.org/10.5194/acp-23-10795-2023, https://doi.org/10.5194/acp-23-10795-2023, 2023
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Particle uptakes of HCHO and the impacts on PM2.5 and O3 production remain highly uncertain. Based on the investigation of co-occurring wintertime O3 and PM2.5 pollution in a coastal city of southeast China, we found enhanced heterogeneous formation of hydroxymethanesulfonate (HMS) and increased ROx concentrations and net O3 production rates. The findings of this study are helpful to better explore the mechanisms of key precursors for co-occurring PM2.5 and O3 pollution.
Foteini Stavropoulou, Katarina Vinković, Bert Kers, Marcel de Vries, Steven van Heuven, Piotr Korbeń, Martina Schmidt, Julia Wietzel, Pawel Jagoda, Jaroslav M. Necki, Jakub Bartyzel, Hossein Maazallahi, Malika Menoud, Carina van der Veen, Sylvia Walter, Béla Tuzson, Jonas Ravelid, Randulph Paulo Morales, Lukas Emmenegger, Dominik Brunner, Michael Steiner, Arjan Hensen, Ilona Velzeboer, Pim van den Bulk, Hugo Denier van der Gon, Antonio Delre, Maklawe Essonanawe Edjabou, Charlotte Scheutz, Marius Corbu, Sebastian Iancu, Denisa Moaca, Alin Scarlat, Alexandru Tudor, Ioana Vizireanu, Andreea Calcan, Magdalena Ardelean, Sorin Ghemulet, Alexandru Pana, Aurel Constantinescu, Lucian Cusa, Alexandru Nica, Calin Baciu, Cristian Pop, Andrei Radovici, Alexandru Mereuta, Horatiu Stefanie, Alexandru Dandocsi, Bas Hermans, Stefan Schwietzke, Daniel Zavala-Araiza, Huilin Chen, and Thomas Röckmann
Atmos. Chem. Phys., 23, 10399–10412, https://doi.org/10.5194/acp-23-10399-2023, https://doi.org/10.5194/acp-23-10399-2023, 2023
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In this study, we quantify CH4 emissions from onshore oil production sites in Romania at source and facility level using a combination of ground- and drone-based measurement techniques. We show that the total CH4 emissions in our studied areas are much higher than the emissions reported to UNFCCC, and up to three-quarters of the detected emissions are related to operational venting. Our results suggest that oil and gas production infrastructure in Romania holds a massive mitigation potential.
Chunxiang Ye, Shuzheng Guo, Weili Lin, Fangjie Tian, Jianshu Wang, Chong Zhang, Suzhen Chi, Yi Chen, Yingjie Zhang, Limin Zeng, Xin Li, Duo Bu, Jiacheng Zhou, and Weixiong Zhao
Atmos. Chem. Phys., 23, 10383–10397, https://doi.org/10.5194/acp-23-10383-2023, https://doi.org/10.5194/acp-23-10383-2023, 2023
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Online volatile organic compound (VOC) measurements by gas chromatography–mass spectrometry, with other O3 precursors, were used to identify key VOC and other key sources in Lhasa. Total VOCs (TVOCs), alkanes, and aromatics are half as abundant as in Beijing. Oxygenated VOCs (OVOCs) consist of 52 % of the TVOCs. Alkenes and OVOCs account for 80 % of the ozone formation potential. Aromatics dominate secondary organic aerosol potential. Positive matrix factorization decomposed residential sources.
Brandon Bottorff, Michelle M. Lew, Youngjun Woo, Pamela Rickly, Matthew D. Rollings, Benjamin Deming, Daniel C. Anderson, Ezra Wood, Hariprasad D. Alwe, Dylan B. Millet, Andrew Weinheimer, Geoff Tyndall, John Ortega, Sebastien Dusanter, Thierry Leonardis, James Flynn, Matt Erickson, Sergio Alvarez, Jean C. Rivera-Rios, Joshua D. Shutter, Frank Keutsch, Detlev Helmig, Wei Wang, Hannah M. Allen, Johnathan H. Slade, Paul B. Shepson, Steven Bertman, and Philip S. Stevens
Atmos. Chem. Phys., 23, 10287–10311, https://doi.org/10.5194/acp-23-10287-2023, https://doi.org/10.5194/acp-23-10287-2023, 2023
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The hydroxyl (OH), hydroperoxy (HO2), and organic peroxy (RO2) radicals play important roles in atmospheric chemistry and have significant air quality implications. Here, we compare measurements of OH, HO2, and total peroxy radicals (XO2) made in a remote forest in Michigan, USA, to predictions from a series of chemical models. Lower measured radical concentrations suggest that the models may be missing an important radical sink and overestimating the rate of ozone production in this forest.
Jenny Oh, Chubashini Shunthirasingham, Ying Duan Lei, Faqiang Zhan, Yuening Li, Abigaëlle Dalpé Castilloux, Amina Ben Chaaben, Zhe Lu, Kelsey Lee, Frank A. P. C. Gobas, Sabine Eckhardt, Nick Alexandrou, Hayley Hung, and Frank Wania
Atmos. Chem. Phys., 23, 10191–10205, https://doi.org/10.5194/acp-23-10191-2023, https://doi.org/10.5194/acp-23-10191-2023, 2023
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An emerging brominated flame retardant (BFR) called TBECH (1,2-dibromo-4-(1,2-dibromoethyl)cyclohexane) has never been produced or imported for use in Canada yet is found to be one of the most abundant gaseous BFRs in the Canadian atmosphere. The recorded spatial and temporal variability of TBECH suggest that the release from imported consumer products containing TBECH is the most likely explanation for its environmental occurrence in Canada.
Olivia E. Clifton, Donna Schwede, Christian Hogrefe, Jesse O. Bash, Sam Bland, Philip Cheung, Mhairi Coyle, Lisa Emberson, Johannes Flemming, Erick Fredj, Stefano Galmarini, Laurens Ganzeveld, Orestis Gazetas, Ignacio Goded, Christopher D. Holmes, László Horváth, Vincent Huijnen, Qian Li, Paul A. Makar, Ivan Mammarella, Giovanni Manca, J. William Munger, Juan L. Pérez-Camanyo, Jonathan Pleim, Limei Ran, Roberto San Jose, Sam J. Silva, Ralf Staebler, Shihan Sun, Amos P. K. Tai, Eran Tas, Timo Vesala, Tamás Weidinger, Zhiyong Wu, and Leiming Zhang
Atmos. Chem. Phys., 23, 9911–9961, https://doi.org/10.5194/acp-23-9911-2023, https://doi.org/10.5194/acp-23-9911-2023, 2023
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A primary sink of air pollutants is dry deposition. Dry deposition estimates differ across the models used to simulate atmospheric chemistry. Here, we introduce an effort to examine dry deposition schemes from atmospheric chemistry models. We provide our approach’s rationale, document the schemes, and describe datasets used to drive and evaluate the schemes. We also launch the analysis of results by evaluating against observations and identifying the processes leading to model–model differences.
Qindan Zhu, Bryan Place, Eva Y. Pfannerstill, Sha Tong, Huanxin Zhang, Jun Wang, Clara M. Nussbaumer, Paul Wooldridge, Benjamin C. Schulze, Caleb Arata, Anthony Bucholtz, John H. Seinfeld, Allen H. Goldstein, and Ronald C. Cohen
Atmos. Chem. Phys., 23, 9669–9683, https://doi.org/10.5194/acp-23-9669-2023, https://doi.org/10.5194/acp-23-9669-2023, 2023
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Nitrogen oxide (NOx) is a hazardous air pollutant, and it is the precursor of short-lived climate forcers like tropospheric ozone and aerosol particles. While NOx emissions from transportation has been strictly regulated, soil NOx emissions are overlooked. We use the airborne flux measurements to observe NOx emissions from highways and urban and cultivated soil land cover types. We show non-negligible soil NOx emissions, which are significantly underestimated in current model simulations.
Xin Yang, Kimberly Strong, Alison Criscitiello, Marta Santos-Garcia, Kristof Bognar, Xiaoyi Zhao, Pierre Fogal, Kaley Walker, Sara Morris, and Peter Effertz
EGUsphere, https://doi.org/10.5194/egusphere-2023-1446, https://doi.org/10.5194/egusphere-2023-1446, 2023
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This study uses in-situ field data collected from a Canadian high Arctic site to demonstrate that surface snow in early spring is a net sink of atmospheric bromine and nitrogen. In addition, surface snow bromide and nitrate are significantly correlated, one molecule bromide deposited is accompanied by 4–7 molecules nitrate, indicating the oxidation of reactive nitrogen is accelerated by reactive bromine. This is the first time such an effect was seen in snow chemistry on a time scale of one day.
Money Ossohou, Jonathan Edward Hickman, Lieven Clarisse, Pierre-François Coheur, Martin Van Damme, Marcellin Adon, Véronique Yoboué, Eric Gardrat, Maria Dias Alvès, and Corinne Galy-Lacaux
Atmos. Chem. Phys., 23, 9473–9494, https://doi.org/10.5194/acp-23-9473-2023, https://doi.org/10.5194/acp-23-9473-2023, 2023
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The updated analyses of ground-based concentrations and satellite total vertical columns of atmospheric ammonia help us to better understand 21st century ammonia dynamics in sub-Saharan Africa. We conclude that the drivers of trends are agriculture in the dry savanna of Katibougou, Mali; air temperature and agriculture in the wet savanna of Djougou, Benin, and Lamto, Côte d'Ivoire; and leaf area index, air temperature, residential, and agriculture in forests of Bomassa, Republic of Congo.
Hyeri Park, Jooil Kim, Haklim Choi, Sohyeon Geum, Yeaseul Kim, Rona L. Thompson, Jens Mühle, Peter K. Salameh, Christina M. Harth, Kieran M. Stanley, Simon O'Doherty, Paul J. Fraser, Peter G. Simmonds, Paul B. Krummel, Ray F. Weiss, Ronald G. Prinn, and Sunyoung Park
Atmos. Chem. Phys., 23, 9401–9411, https://doi.org/10.5194/acp-23-9401-2023, https://doi.org/10.5194/acp-23-9401-2023, 2023
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Based on atmospheric HFC-23 observations, the first estimate of post-CDM HFC-23 emissions in eastern Asia for 2008–2019 shows that these emissions contribute significantly to the global emissions rise. The observation-derived emissions were much larger than the bottom-up estimates expected to approach zero after 2015 due to national abatement activities. These discrepancies could be attributed to unsuccessful factory-level HFC-23 abatement and inaccurate quantification of emission reductions.
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