Articles | Volume 10, issue 6
https://doi.org/10.5194/bg-10-4241-2013
© Author(s) 2013. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/bg-10-4241-2013
© Author(s) 2013. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Seasonal measurements of total OH reactivity emission rates from Norway spruce in 2011
A.C. Nölscher
Department of Atmospheric Chemistry, Max Planck Institute for Chemistry, Mainz, Germany
E. Bourtsoukidis
Institute for Atmospheric and Environmental Sciences, J.W. Goethe University, Frankfurt/Main, Germany
International Max Planck Research School for Atmospheric Chemistry and Physics, Max Planck Institute for Chemistry, Mainz, Germany
B. Bonn
Institute for Atmospheric and Environmental Sciences, J.W. Goethe University, Frankfurt/Main, Germany
J. Kesselmeier
Department of Biogeochemistry, Max Planck Institute for Chemistry, Mainz, Germany
J. Lelieveld
Department of Atmospheric Chemistry, Max Planck Institute for Chemistry, Mainz, Germany
J. Williams
Department of Atmospheric Chemistry, Max Planck Institute for Chemistry, Mainz, Germany
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Composite analysis of gas concentration before and after rainfall, during the day and night, gives insight into the complex relationship between trace gas variability and precipitation. The analysis helps us 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.
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We evaluated the performance of four cascade impactors for collecting and analyzing organic markers in airborne UFP under laboratory and field conditions. The cut-off was influenced by both impactor design and aerosol mixture. Two key factors caused variations in mass concentrations: evaporation of semi-volatile compounds and bounce of larger particles and fragments. Our findings highlight the complexities of accurately separating and analyzing organic marker mass concentrations in airborne UFP.
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Atmos. Meas. Tech., 17, 4553–4579, https://doi.org/10.5194/amt-17-4553-2024, https://doi.org/10.5194/amt-17-4553-2024, 2024
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We constructed and characterized a new indoor Teflon atmospheric simulation chamber. We evaluated wall losses, photolysis rates, and secondary reactions of multifunctional photooxidation products in the chamber. To measure these products on-line, we combined chromatographic and mass spectrometric analyses to obtain both isomeric information and a high temporal resolution. For method validation, we studied the formation yields of the main ring-retaining products of toluene.
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Here, we study the transport of ultrafine particles (UFPs) from an airport to two new adjacent measuring sites for 1 year. The number of UFPs in the air and the diurnal variation are typical urban. Winds from the airport show increased number concentrations. Additionally, considering wind frequencies, we estimate that, from all UFPs measured at the two sites, 10 %–14 % originate from the airport and/or other UFP sources from between the airport and site.
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Incomplete mixing (segregation) results in reduced chemical reaction rates compared to those expected from mean values and rate constants. Segregation has been suggested to cause discrepancies between modelled and measured OH radical concentrations. In this work, we summarize the intensities of segregation for the reaction of OH and isoprene for different field and modelling studies and compare those to our results from measurements in a pristine environment.
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.
Ana María Yáñez-Serrano, Anke Christine Nölscher, Efstratios Bourtsoukidis, Eliane Gomes Alves, Laurens Ganzeveld, Boris Bonn, Stefan Wolff, Marta Sa, Marcia Yamasoe, Jonathan Williams, Meinrat O. Andreae, and Jürgen Kesselmeier
Atmos. Chem. Phys., 18, 3403–3418, https://doi.org/10.5194/acp-18-3403-2018, https://doi.org/10.5194/acp-18-3403-2018, 2018
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Yudong Yang, Min Shao, Stephan Keßel, Yue Li, Keding Lu, Sihua Lu, Jonathan Williams, Yuanhang Zhang, Liming Zeng, Anke C. Nölscher, Yusheng Wu, Xuemei Wang, and Junyu Zheng
Atmos. Chem. Phys., 17, 7127–7142, https://doi.org/10.5194/acp-17-7127-2017, https://doi.org/10.5194/acp-17-7127-2017, 2017
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Total OH reactivity is an important parameter to evaluate understanding of atmospheric chemistry, especially the VOC contribution to air pollution. Measured by comparative reactivity methods, total OH reactivity in Beijing and Heshan revealed significant differences between measured and calculated results, such as missing reactivity, which were related to unmeasured primary or secondary species. This missing reactivity would introduce a 21–30 % underestimation for ozone production efficiency.
A. M. Yáñez-Serrano, A. C. Nölscher, E. Bourtsoukidis, B. Derstroff, N. Zannoni, V. Gros, M. Lanza, J. Brito, S. M. Noe, E. House, C. N. Hewitt, B. Langford, E. Nemitz, T. Behrendt, J. Williams, P. Artaxo, M. O. Andreae, and J. Kesselmeier
Atmos. Chem. Phys., 16, 10965–10984, https://doi.org/10.5194/acp-16-10965-2016, https://doi.org/10.5194/acp-16-10965-2016, 2016
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This paper provides a general overview of methyl ethyl ketone (MEK) ambient observations in different ecosystems around the world in order to provide insights into the sources, sink and role of MEK in the atmosphere.
M. O. Andreae, O. C. Acevedo, A. Araùjo, P. Artaxo, C. G. G. Barbosa, H. M. J. Barbosa, J. Brito, S. Carbone, X. Chi, B. B. L. Cintra, N. F. da Silva, N. L. Dias, C. Q. Dias-Júnior, F. Ditas, R. Ditz, A. F. L. Godoi, R. H. M. Godoi, M. Heimann, T. Hoffmann, J. Kesselmeier, T. Könemann, M. L. Krüger, J. V. Lavric, A. O. Manzi, A. P. Lopes, D. L. Martins, E. F. Mikhailov, D. Moran-Zuloaga, B. W. Nelson, A. C. Nölscher, D. Santos Nogueira, M. T. F. Piedade, C. Pöhlker, U. Pöschl, C. A. Quesada, L. V. Rizzo, C.-U. Ro, N. Ruckteschler, L. D. A. Sá, M. de Oliveira Sá, C. B. Sales, R. M. N. dos Santos, J. Saturno, J. Schöngart, M. Sörgel, C. M. de Souza, R. A. F. de Souza, H. Su, N. Targhetta, J. Tóta, I. Trebs, S. Trumbore, A. van Eijck, D. Walter, Z. Wang, B. Weber, J. Williams, J. Winderlich, F. Wittmann, S. Wolff, and A. M. Yáñez-Serrano
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D. Mogensen, R. Gierens, J. N. Crowley, P. Keronen, S. Smolander, A. Sogachev, A. C. Nölscher, L. Zhou, M. Kulmala, M. J. Tang, J. Williams, and M. Boy
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A. M. Yáñez-Serrano, A. C. Nölscher, J. Williams, S. Wolff, E. Alves, G. A. Martins, E. Bourtsoukidis, J. Brito, K. Jardine, P. Artaxo, and J. Kesselmeier
Atmos. Chem. Phys., 15, 3359–3378, https://doi.org/10.5194/acp-15-3359-2015, https://doi.org/10.5194/acp-15-3359-2015, 2015
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
A. C. Nölscher, V. Sinha, S. Bockisch, T. Klüpfel, and J. Williams
Atmos. Meas. Tech., 5, 2981–2992, https://doi.org/10.5194/amt-5-2981-2012, https://doi.org/10.5194/amt-5-2981-2012, 2012
Laura Wüst, Patrick Dewald, Gunther N. T. E. Türk, Jos Lelieveld, and John N. Crowley
EGUsphere, https://doi.org/10.5194/egusphere-2024-3694, https://doi.org/10.5194/egusphere-2024-3694, 2024
This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
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Detection of NO2 via cavity ring-down spectroscopy (CRDS) after thermal dissociation (TD) of alkyl and peroxy nitrates can be used to detect total atmospheric organic nitrates originating from the interaction between biogenic emissions of volatile organic compounds and nitrogen oxides of anthropogenic origin. Here we present an improved TD-CRDS which avoids systematic bias resulting from secondary chemistry in the heated inlets and which can be deployed in regions with strong biogenic emissions.
Simone T. Andersen, Rolf Sander, Patrick Dewald, Laura Wüst, Tobias Seubert, Gunther N. T. E. Türk, Jan Schuladen, Max R. McGillen, Chaoyang Xue, Abdelwahid Mellouki, Alexandre Kukui, Vincent Michoud, Manuela Cirtog, Mathieu Cazaunau, Astrid Bauville, Hichem Bouzidi, Paola Formenti, Cyrielle Denjean, Jean-Claude Etienne, Olivier Garrouste, Christopher Cantrell, Jos Lelieveld, and John N. Crowley
EGUsphere, https://doi.org/10.5194/egusphere-2024-3437, https://doi.org/10.5194/egusphere-2024-3437, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Measurements and modelling of reactive nitrogen gases observed in a suburban temperate forest in Rambouillet, France circa 50 km southwest of Paris in 2022 indicate that the biosphere rapidly scavenges organic nitrates of mixed biogenic and anthropogenic origin, resulting in short lifetimes for e.g. alkyl nitrates and peroxy nitrates.
Akima Ringsdorf, Achim Edtbauer, Bruna Holanda, Christopher Poehlker, Marta O. Sá, Alessandro Araújo, Jürgen Kesselmeier, Jos Lelieveld, and Jonathan Williams
Atmos. Chem. Phys., 24, 11883–11910, https://doi.org/10.5194/acp-24-11883-2024, https://doi.org/10.5194/acp-24-11883-2024, 2024
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We show the average height distribution of separately observed aldehydes and ketones over a day and discuss their rainforest-specific sources and sinks as well as their seasonal changes above the Amazon. Ketones have much longer atmospheric lifetimes than aldehydes and thus different implications for atmospheric chemistry. However, they are commonly observed together, which we overcome by measuring with a NO+ chemical ionization mass spectrometer for the first time in the Amazon rainforest.
Simone T. Andersen, Max R. McGillen, Chaoyang Xue, Tobias Seubert, Patrick Dewald, Gunther N. T. E. Türk, Jan Schuladen, Cyrielle Denjean, Jean-Claude Etienne, Olivier Garrouste, Marina Jamar, Sergio Harb, Manuela Cirtog, Vincent Michoud, Mathieu Cazaunau, Antonin Bergé, Christopher Cantrell, Sebastien Dusanter, Bénédicte Picquet-Varrault, Alexandre Kukui, Abdelwahid Mellouki, Lucy J. Carpenter, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 24, 11603–11618, https://doi.org/10.5194/acp-24-11603-2024, https://doi.org/10.5194/acp-24-11603-2024, 2024
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Using measurements of various trace gases in a suburban forest near Paris in the summer of 2022, we were able to gain insight into the sources and sinks of NOx (NO+NO2) with a special focus on their nighttime chemical and physical loss processes. NO was observed as a result of nighttime soil emissions when O3 levels were strongly depleted by deposition. NO oxidation products were not observed at night, indicating that soil and/or foliar surfaces are an efficient sink of reactive N.
Pantelis Georgiades, Theo Economou, Yiannis Proestos, Jose Araya, Jos Lelieveld, and Marco Neira
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2024-344, https://doi.org/10.5194/essd-2024-344, 2024
Revised manuscript under review for ESSD
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Climate change is posing increasing challenges in the dairy cattle farming sector, as heat stress adversely affects the animals' health and milk production. To accurately asses these impacts, we developed a machine learning model to downscale daily climate data to hourly Temperature Humidity Index (THI) values. We utilised historical weather data to train our model and applied it to future climate projections, under two climate scenarios.
Patrick Dewald, Tobias Seubert, Simone T. Andersen, Gunther N. T. E. Türk, Jan Schuladen, Max R. McGillen, Cyrielle Denjean, Jean-Claude Etienne, Olivier Garrouste, Marina Jamar, Sergio Harb, Manuela Cirtog, Vincent Michoud, Mathieu Cazaunau, Antonin Bergé, Christopher Cantrell, Sebastien Dusanter, Bénédicte Picquet-Varrault, Alexandre Kukui, Chaoyang Xue, Abdelwahid Mellouki, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 24, 8983–8997, https://doi.org/10.5194/acp-24-8983-2024, https://doi.org/10.5194/acp-24-8983-2024, 2024
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In the scope of a field campaign in a suburban forest near Paris in the summer of 2022, we measured the reactivity of the nitrate radical NO3 towards biogenic volatile organic compounds (BVOCs; e.g. monoterpenes) mainly below but also above the canopy. NO3 reactivity was the highest during nights with strong temperature inversions and decreased strongly with height. Reactions with BVOCs were the main removal process of NO3 throughout the diel cycle below the canopy.
Luiz A. T. Machado, Jürgen Kesselmeier, Santiago Botía, Hella van Asperen, Meinrat O. Andreae, Alessandro C. de Araújo, Paulo Artaxo, Achim Edtbauer, Rosaria R. Ferreira, Marco A. Franco, Hartwig Harder, Sam P. Jones, Cléo Q. Dias-Júnior, Guido G. Haytzmann, Carlos A. Quesada, Shujiro Komiya, Jost Lavric, Jos Lelieveld, Ingeborg Levin, Anke Nölscher, Eva Pfannerstill, Mira L. 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
Atmos. Chem. Phys., 24, 8893–8910, https://doi.org/10.5194/acp-24-8893-2024, https://doi.org/10.5194/acp-24-8893-2024, 2024
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Composite analysis of gas concentration before and after rainfall, during the day and night, gives insight into the complex relationship between trace gas variability and precipitation. The analysis helps us 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.
Elisabeth Eckenberger, Andreas Mittereder, Nadine Gawlitta, Jürgen Schnelle-Kreis, Martin Sklorz, Dieter Brüggemann, Ralf Zimmermann, and Anke Christine Nölscher
Aerosol Research Discuss., https://doi.org/10.5194/ar-2024-20, https://doi.org/10.5194/ar-2024-20, 2024
Revised manuscript accepted for AR
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We evaluated the performance of four cascade impactors for collecting and analyzing organic markers in airborne UFP under laboratory and field conditions. The cut-off was influenced by both impactor design and aerosol mixture. Two key factors caused variations in mass concentrations: evaporation of semi-volatile compounds and bounce of larger particles and fragments. Our findings highlight the complexities of accurately separating and analyzing organic marker mass concentrations in airborne UFP.
Pantelis Georgiades, Matthias Kohl, Mihalis A. Nicolaou, Theodoros Christoudias, Andrea Pozzer, Constantine Dovrolis, and Jos Lelieveld
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2024-314, https://doi.org/10.5194/essd-2024-314, 2024
Manuscript not accepted for further review
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This study maps global ultrafine particle (UFP) concentrations, pollutants known to affect health, using machine learning. By combining environmental and urban data, we predicted UFP levels at a fine 1 km resolution, highlighting areas of high exposure. Our results provide data for public health policies aimed at reducing air pollution impacts. This research bridges data gaps, offering a valuable tool for understanding and mitigating the health effects of UFP exposure.
Finja Löher, Esther Borrás, Amalia Muñoz, and Anke Christine Nölscher
Atmos. Meas. Tech., 17, 4553–4579, https://doi.org/10.5194/amt-17-4553-2024, https://doi.org/10.5194/amt-17-4553-2024, 2024
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We constructed and characterized a new indoor Teflon atmospheric simulation chamber. We evaluated wall losses, photolysis rates, and secondary reactions of multifunctional photooxidation products in the chamber. To measure these products on-line, we combined chromatographic and mass spectrometric analyses to obtain both isomeric information and a high temporal resolution. For method validation, we studied the formation yields of the main ring-retaining products of toluene.
Anna Martin, Veronika Gayler, Benedikt Steil, Klaus Klingmüller, Patrick Jöckel, Holger Tost, Jos Lelieveld, and Andrea Pozzer
Geosci. Model Dev., 17, 5705–5732, https://doi.org/10.5194/gmd-17-5705-2024, https://doi.org/10.5194/gmd-17-5705-2024, 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 using different datasets, the coupled model shows strong correlations of key variables, such as land surface temperature, surface albedo and radiation flux. The versatility of the model increases significantly, while the overall performance does not degrade.
Ryan Vella, Matthew Forrest, Andrea Pozzer, Alexandra P. Tsimpidi, Thomas Hickler, Jos Lelieveld, and Holger Tost
EGUsphere, https://doi.org/10.5194/egusphere-2024-2014, https://doi.org/10.5194/egusphere-2024-2014, 2024
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This study examines how land cover changes influence biogenic volatile organic compound (BVOC) emissions and atmospheric states. Using a coupled chemistry-climate/vegetation model, we compare present-day land cover (deforested for crops and grazing) with natural vegetation, and an extreme reforestation scenario. We find that vegetation changes significantly impact global BVOC emissions and organic aerosols but have a relatively small effect on total aerosols, clouds, and radiative effects.
Georgia Lazoglou, Theo Economou, Christina Anagnostopoulou, George Zittis, Anna Tzyrkalli, Pantelis Georgiades, and Jos Lelieveld
Geosci. Model Dev., 17, 4689–4703, https://doi.org/10.5194/gmd-17-4689-2024, https://doi.org/10.5194/gmd-17-4689-2024, 2024
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This study focuses 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 are applied and rigorously evaluated. These results are encouraging for using the multivariate machine learning method random forest to increase the accuracy of climate models concerning the projection of the number of wet days.
Linda Ort, Lenard Lukas Röder, Uwe Parchatka, Rainer Königstedt, Daniel Crowley, Frank Kunz, Ralf Wittkowski, Jos Lelieveld, and Horst Fischer
Atmos. Meas. Tech., 17, 3553–3565, https://doi.org/10.5194/amt-17-3553-2024, https://doi.org/10.5194/amt-17-3553-2024, 2024
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Airborne in situ measurements are of great importance to collect valuable data to improve our knowledge of the atmosphere but also present 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 in-flight 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.
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.
Julius Seidler, Markus N. Friedrich, Christoph K. Thomas, and Anke C. Nölscher
Atmos. Chem. Phys., 24, 137–153, https://doi.org/10.5194/acp-24-137-2024, https://doi.org/10.5194/acp-24-137-2024, 2024
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Here, we study the transport of ultrafine particles (UFPs) from an airport to two new adjacent measuring sites for 1 year. The number of UFPs in the air and the diurnal variation are typical urban. Winds from the airport show increased number concentrations. Additionally, considering wind frequencies, we estimate that, from all UFPs measured at the two sites, 10 %–14 % originate from the airport and/or other UFP sources from between the airport and site.
Ryan Vella, Andrea Pozzer, Matthew Forrest, Jos Lelieveld, Thomas Hickler, and Holger Tost
Biogeosciences, 20, 4391–4412, https://doi.org/10.5194/bg-20-4391-2023, https://doi.org/10.5194/bg-20-4391-2023, 2023
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We investigated the effect of the El Niño–Southern Oscillation (ENSO) on biogenic volatile organic compound (BVOC) emissions from plants. ENSO events can cause a significant increase in these emissions, which have a long-term impact on the Earth's atmosphere. Persistent ENSO conditions can cause long-term changes in vegetation, resulting in even higher BVOC emissions. We link ENSO-induced emission anomalies with driving atmospheric and vegetational variables.
Susanna Strada, Andrea Pozzer, Graziano Giuliani, Erika Coppola, Fabien Solmon, Xiaoyan Jiang, Alex Guenther, Efstratios Bourtsoukidis, Dominique Serça, Jonathan Williams, and Filippo Giorgi
Atmos. Chem. Phys., 23, 13301–13327, https://doi.org/10.5194/acp-23-13301-2023, https://doi.org/10.5194/acp-23-13301-2023, 2023
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Water deficit modifies emissions of isoprene, an aromatic compound released by plants that influences the production of an air pollutant such as ozone. Numerical modelling shows that, during the warmest and driest summers, isoprene decreases between −20 and −60 % over the Euro-Mediterranean region, while near-surface ozone only diminishes by a few percent. Decreases in isoprene emissions not only happen under dry conditions, but also could occur after prolonged or repeated water deficits.
Zaneta Hamryszczak, Antonia Hartmann, Dirk Dienhart, Sascha Hafermann, Bettina Brendel, Rainer Königstedt, Uwe Parchatka, Jos Lelieveld, and Horst Fischer
Atmos. Meas. Tech., 16, 4741–4756, https://doi.org/10.5194/amt-16-4741-2023, https://doi.org/10.5194/amt-16-4741-2023, 2023
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Hydroperoxide measurements improve the understanding of atmospheric oxidation processes. We introduce an instrumental setup for airborne measurements. The aim of the work is the characterization of the measurement method with emphasis on interferences impacting instrumental uncertainty. Technical and physical challenges do not critically impact the instrumental performance. The instrument resolves dynamic processes, such as convective transport, as shown based on the CAFE-Brazil campaign.
Matthias Kohl, Jos Lelieveld, Sourangsu Chowdhury, Sebastian Ehrhart, Disha Sharma, Yafang Cheng, Sachchida Nand Tripathi, Mathew Sebastian, Govindan Pandithurai, Hongli Wang, and Andrea Pozzer
Atmos. Chem. Phys., 23, 13191–13215, https://doi.org/10.5194/acp-23-13191-2023, https://doi.org/10.5194/acp-23-13191-2023, 2023
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Knowledge on atmospheric ultrafine particles (UFPs) with a diameter smaller than 100 nm is crucial for public health and the hydrological cycle. We present a new global dataset of UFP concentrations at the Earth's surface derived with a comprehensive chemistry–climate model and evaluated with ground-based observations. The evaluation results are combined with high-resolution primary emissions to downscale UFP concentrations to an unprecedented horizontal resolution of 0.1° × 0.1°.
Clara M. Nussbaumer, 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.
Eliane Gomes Alves, Raoni Aquino Santana, Cléo Quaresma Dias-Júnior, Santiago Botía, Tyeen Taylor, Ana Maria Yáñez-Serrano, Jürgen Kesselmeier, Efstratios Bourtsoukidis, Jonathan Williams, Pedro Ivo Lembo Silveira de Assis, Giordane Martins, Rodrigo de Souza, Sérgio Duvoisin Júnior, Alex Guenther, Dasa Gu, Anywhere Tsokankunku, Matthias Sörgel, Bruce Nelson, Davieliton Pinto, Shujiro Komiya, Diogo Martins Rosa, Bettina Weber, Cybelli Barbosa, Michelle Robin, Kenneth J. Feeley, Alvaro Duque, Viviana Londoño Lemos, Maria Paula Contreras, Alvaro Idarraga, Norberto López, Chad Husby, Brett Jestrow, and Iván Mauricio Cely Toro
Atmos. Chem. Phys., 23, 8149–8168, https://doi.org/10.5194/acp-23-8149-2023, https://doi.org/10.5194/acp-23-8149-2023, 2023
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Isoprene is emitted mainly by plants and can influence atmospheric chemistry and air quality. But, there are uncertainties in model emission estimates and follow-up atmospheric processes. In our study, with long-term observational datasets of isoprene and biological and environmental factors from central Amazonia, we show that isoprene emission estimates could be improved when biological processes were mechanistically incorporated into the model.
Seyed Omid Nabavi, Theodoros Christoudias, Yiannis Proestos, Christos Fountoukis, Huda Al-Sulaiti, and Jos Lelieveld
Atmos. Chem. Phys., 23, 7719–7739, https://doi.org/10.5194/acp-23-7719-2023, https://doi.org/10.5194/acp-23-7719-2023, 2023
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The objective of our study is to comprehensively assess the timing of radioactive material transportation and deposition, along with the associated population exposure in the designated region. We employed diverse meteorological inputs, emission specifics, and simulation codes, aiming to quantify the level of uncertainty.
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.
Lisa Ernle, Monika Akima Ringsdorf, and Jonathan Williams
Atmos. Meas. Tech., 16, 1179–1194, https://doi.org/10.5194/amt-16-1179-2023, https://doi.org/10.5194/amt-16-1179-2023, 2023
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Atmospheric ozone can induce artefacts in volatile organic compound measurements. Laboratory tests were made using GC-MS and PTR-MS aircraft systems under tropospheric and stratospheric conditions of humidity and ozone, with and without sodium thiosulfate filter scrubbers. Ozone in dry air produces some carbonyls and degrades alkenes. The scrubber lifetime depends on ozone concentration, flow rate and humidity. For the troposphere with scrubber, no significant artefacts were found over 14 d.
Lenard L. Röder, Patrick Dewald, Clara M. Nussbaumer, Jan Schuladen, John N. Crowley, Jos Lelieveld, and Horst Fischer
Atmos. Meas. Tech., 16, 1167–1178, https://doi.org/10.5194/amt-16-1167-2023, https://doi.org/10.5194/amt-16-1167-2023, 2023
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Field experiments in atmospheric chemistry provide insights into chemical interactions of our atmosphere. However, high data coverage and accuracy are needed to enable further analysis. In this study, we explore a statistical method that combines knowledge about the chemical reactions with information from measurements to increase the quality of field experiment datasets. We test the algorithm for several applications and discuss limitations that depend on the specific variable and the dynamics.
Ryan Vella, Matthew Forrest, Jos Lelieveld, and Holger Tost
Geosci. Model Dev., 16, 885–906, https://doi.org/10.5194/gmd-16-885-2023, https://doi.org/10.5194/gmd-16-885-2023, 2023
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Biogenic volatile organic compounds (BVOCs) are released by vegetation and have a major impact on atmospheric chemistry and aerosol formation. Non-interacting vegetation constrains the majority of numerical models used to estimate global BVOC emissions, and thus, the effects of changing vegetation on emissions are not addressed. In this work, we replace the offline vegetation with dynamic vegetation states by linking a chemistry–climate model with a global dynamic vegetation model.
Jennifer Schallock, Christoph Brühl, Christine Bingen, Michael Höpfner, Landon Rieger, and Jos Lelieveld
Atmos. Chem. Phys., 23, 1169–1207, https://doi.org/10.5194/acp-23-1169-2023, https://doi.org/10.5194/acp-23-1169-2023, 2023
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We characterized the influence of volcanic aerosols for the period 1990–2019 and established a volcanic SO2 emission inventory that includes more than 500 eruptions. From limb-based satellite observations of SO2 and extinction, we derive 3D plumes of SO2 perturbations and injected mass by a novel method. We calculate instantaneous radiative forcing with a comprehensive chemisty climate model. Our results show that smaller eruptions can also contribute to the stratospheric aerosol forcing.
Denis Leppla, Nora Zannoni, Leslie Kremper, Jonathan Williams, Christopher Pöhlker, Marta Sá, Maria Christina Solci, and Thorsten Hoffmann
Atmos. Chem. Phys., 23, 809–820, https://doi.org/10.5194/acp-23-809-2023, https://doi.org/10.5194/acp-23-809-2023, 2023
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Chiral chemodiversity plays a critical role in biochemical processes such as insect and plant communication. Here we report on the measurement of chiral-specified secondary organic aerosol in the Amazon rainforest. The results show that the chiral ratio is mainly determined by large-scale emission processes. Characteristic emissions of chiral aerosol precursors from different forest ecosystems can thus provide large-scale information on different biogenic sources via chiral particle analysis.
Mohamed Abdelkader, Georgiy Stenchikov, Andrea Pozzer, Holger Tost, and Jos Lelieveld
Atmos. Chem. Phys., 23, 471–500, https://doi.org/10.5194/acp-23-471-2023, https://doi.org/10.5194/acp-23-471-2023, 2023
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We study the effect of injected volcanic ash, water vapor, and SO2 on the development of the volcanic cloud and the stratospheric aerosol optical depth (AOD). Both are sensitive to the initial injection height and to the aging of the volcanic ash shaped by heterogeneous chemistry coupled with the ozone cycle. The paper explains the large differences in AOD for different injection scenarios, which could improve the estimate of the radiative forcing of volcanic eruptions.
Dirk Dienhart, Bettina Brendel, John N. Crowley, Philipp G. Eger, Hartwig Harder, Monica Martinez, Andrea Pozzer, Roland Rohloff, Jan Schuladen, Sebastian Tauer, David Walter, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 23, 119–142, https://doi.org/10.5194/acp-23-119-2023, https://doi.org/10.5194/acp-23-119-2023, 2023
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Formaldehyde and hydroperoxide measurements were performed in the marine boundary layer around the Arabian Peninsula and highlight the Suez Canal and Arabian (Persian) Gulf as a hotspot of photochemical air pollution. A comparison with the EMAC model shows that the formaldehyde results match within a factor of 2, while hydrogen peroxide was overestimated by more than a factor of 5, which revealed enhanced HOx (OH+HO2) radicals in the simulation and an underestimation of dry deposition velocites.
Laura Tomsche, Andreas Marsing, Tina Jurkat-Witschas, Johannes Lucke, Stefan Kaufmann, Katharina Kaiser, Johannes Schneider, Monika Scheibe, Hans Schlager, Lenard Röder, Horst Fischer, Florian Obersteiner, Andreas Zahn, Martin Zöger, Jos Lelieveld, and Christiane Voigt
Atmos. Chem. Phys., 22, 15135–15151, https://doi.org/10.5194/acp-22-15135-2022, https://doi.org/10.5194/acp-22-15135-2022, 2022
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The detection of sulfur compounds in the upper troposphere (UT) and lower stratosphere (LS) is a challenge. In-flight measurements of SO2 and sulfate aerosol were performed during the BLUESKY mission in spring 2020 under exceptional atmospheric conditions. Reduced sinks in the dry UTLS and lower but still significant air traffic influenced the enhanced SO2 in the UT, and aged volcanic plumes enhanced the LS sulfate aerosol impacting the atmospheric radiation budget and global climate.
Charlotte M. Beall, Thomas C. J. Hill, Paul J. DeMott, Tobias Köneman, Michael Pikridas, Frank Drewnick, Hartwig Harder, Christopher Pöhlker, Jos Lelieveld, Bettina Weber, Minas Iakovides, Roman Prokeš, Jean Sciare, Meinrat O. Andreae, M. Dale Stokes, and Kimberly A. Prather
Atmos. Chem. Phys., 22, 12607–12627, https://doi.org/10.5194/acp-22-12607-2022, https://doi.org/10.5194/acp-22-12607-2022, 2022
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Ice-nucleating particles (INPs) are rare aerosols that can trigger ice formation in clouds and affect climate-relevant cloud properties such as phase, reflectivity and lifetime. Dust is the dominant INP source, yet few measurements have been reported near major dust sources. We report INP observations within hundreds of kilometers of the biggest dust source regions globally: the Sahara and the Arabian Peninsula. Results show that at temperatures > −15 °C, INPs are dominated by organics.
Mengze Li, Andrea Pozzer, Jos Lelieveld, and Jonathan Williams
Earth Syst. Sci. Data, 14, 4351–4364, https://doi.org/10.5194/essd-14-4351-2022, https://doi.org/10.5194/essd-14-4351-2022, 2022
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We present a northern hemispheric airborne measurement dataset of atmospheric ethane, propane and methane and temporal trends for the time period 2006–2016 in the upper troposphere and lower stratosphere. The growth rates of ethane, methane, and propane in the upper troposphere are -2.24, 0.33, and -0.78 % yr-1, respectively, and in the lower stratosphere they are -3.27, 0.26, and -4.91 % yr-1, respectively, in 2006–2016.
Therese S. Carter, Colette L. Heald, Jesse H. Kroll, Eric C. Apel, Donald Blake, Matthew Coggon, Achim Edtbauer, Georgios Gkatzelis, Rebecca S. Hornbrook, Jeff Peischl, Eva Y. Pfannerstill, Felix Piel, Nina G. Reijrink, Akima Ringsdorf, Carsten Warneke, Jonathan Williams, Armin Wisthaler, and Lu Xu
Atmos. Chem. Phys., 22, 12093–12111, https://doi.org/10.5194/acp-22-12093-2022, https://doi.org/10.5194/acp-22-12093-2022, 2022
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Fires emit many gases which can contribute to smog and air pollution. However, the amount and properties of these chemicals are not well understood, so this work updates and expands their representation in a global atmospheric model, including by adding new chemicals. We confirm that this updated representation generally matches measurements taken in several fire regions. We then show that fires provide ~15 % of atmospheric reactivity globally and more than 75 % over fire source regions.
Simon F. Reifenberg, Anna Martin, Matthias Kohl, Sara Bacer, Zaneta Hamryszczak, Ivan Tadic, Lenard Röder, Daniel J. Crowley, Horst Fischer, Katharina Kaiser, Johannes Schneider, Raphael Dörich, John N. Crowley, Laura Tomsche, Andreas Marsing, Christiane Voigt, Andreas Zahn, Christopher Pöhlker, Bruna A. Holanda, Ovid Krüger, Ulrich Pöschl, Mira Pöhlker, Patrick Jöckel, Marcel Dorf, Ulrich Schumann, Jonathan Williams, Birger Bohn, Joachim Curtius, Hardwig Harder, Hans Schlager, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 22, 10901–10917, https://doi.org/10.5194/acp-22-10901-2022, https://doi.org/10.5194/acp-22-10901-2022, 2022
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In this work we use a combination of observational data from an aircraft campaign and model results to investigate the effect of the European lockdown due to COVID-19 in spring 2020. Using model results, we show that the largest relative changes to the atmospheric composition caused by the reduced emissions are located in the upper troposphere around aircraft cruise altitude, while the largest absolute changes are present at the surface.
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 %.
Patrick Dewald, Clara M. Nussbaumer, Jan Schuladen, Akima Ringsdorf, Achim Edtbauer, Horst Fischer, Jonathan Williams, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 22, 7051–7069, https://doi.org/10.5194/acp-22-7051-2022, https://doi.org/10.5194/acp-22-7051-2022, 2022
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We measured the gas-phase reactivity of the NO3 radical on the summit (825 m a.s.l.) of a semi-rural mountain in southwestern Germany in July 2021. The impact of VOC-induced NO3 losses (mostly monoterpenes) competing with a loss by reaction with NO and photolysis throughout the diel cycle was estimated. Besides chemistry, boundary layer dynamics and plant-physiological processes presumably have a great impact on our observations, which were compared to previous NO3 measurements at the same site.
George K. Georgiou, Theodoros Christoudias, Yiannis Proestos, Jonilda Kushta, Michael Pikridas, Jean Sciare, Chrysanthos Savvides, and Jos Lelieveld
Geosci. Model Dev., 15, 4129–4146, https://doi.org/10.5194/gmd-15-4129-2022, https://doi.org/10.5194/gmd-15-4129-2022, 2022
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We evaluate the skill of the WRF-Chem model to perform high-resolution air quality forecasts (including ozone, nitrogen dioxide, and fine particulate matter) over the Eastern Mediterranean, during winter and summer. We compare the forecast output to observational data from background and urban locations and the forecast output from CAMS. WRF-Chem was found to forecast the concentrations and diurnal profiles of gas-phase pollutants in urban areas with higher accuracy.
Clara M. Nussbaumer, Andrea Pozzer, Ivan Tadic, Lenard Röder, Florian Obersteiner, Hartwig Harder, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 22, 6151–6165, https://doi.org/10.5194/acp-22-6151-2022, https://doi.org/10.5194/acp-22-6151-2022, 2022
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The European COVID-19 lockdowns have significantly reduced the emission of primary pollutants such as NOx, which impacts the tropospheric photochemical processes and the abundance of O3. In this study, we present how the lockdowns have affected tropospheric trace gases and ozone production based on in situ observations and modeling simulations. We additionally show that the chemical regime shifted from a transition point to a NOx limitation in the upper troposphere.
Wenyu Sun, Matias Berasategui, Andrea Pozzer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 22, 4969–4984, https://doi.org/10.5194/acp-22-4969-2022, https://doi.org/10.5194/acp-22-4969-2022, 2022
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The reaction between OH and SO2 is a termolecular process that in the atmosphere results in the formation of H2SO4 and thus aerosols. We present the first temperature- and pressure-dependent measurements of the rate coefficients in N2. This is also the first study to examine the effects of water vapour on the kinetics of this reaction. Our results indicate the rate coefficient is larger than that recommended by evaluation panels, with deviations of up to 30 % in some parts of the atmosphere.
Yanan Zhao, Dennis Booge, Christa A. Marandino, Cathleen Schlundt, Astrid Bracher, Elliot L. Atlas, Jonathan Williams, and Hermann W. Bange
Biogeosciences, 19, 701–714, https://doi.org/10.5194/bg-19-701-2022, https://doi.org/10.5194/bg-19-701-2022, 2022
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We present here, for the first time, simultaneously measured dimethylsulfide (DMS) seawater concentrations and DMS atmospheric mole fractions from the Peruvian upwelling region during two cruises in December 2012 and October 2015. Our results indicate low oceanic DMS concentrations and atmospheric DMS molar fractions in surface waters and the atmosphere, respectively. In addition, the Peruvian upwelling region was identified as an insignificant source of DMS emissions during both periods.
Clara M. Nussbaumer, John N. Crowley, Jan Schuladen, Jonathan Williams, Sascha Hafermann, Andreas Reiffs, Raoul Axinte, Hartwig Harder, Cheryl Ernest, Anna Novelli, Katrin Sala, Monica Martinez, Chinmay Mallik, Laura Tomsche, Christian Plass-Dülmer, Birger Bohn, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 18413–18432, https://doi.org/10.5194/acp-21-18413-2021, https://doi.org/10.5194/acp-21-18413-2021, 2021
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HCHO is an important atmospheric trace gas influencing the photochemical processes in the Earth’s atmosphere, including the budget of HOx and the abundance of tropospheric O3. This research presents the photochemical calculations of HCHO and O3 based on three field campaigns across Europe. We show that HCHO production via the oxidation of only four volatile organic compound precursors, i.e., CH4, CH3CHO, C5H8 and CH3OH, can balance the observed loss at all sites well.
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).
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.
Maria Prass, Meinrat O. Andreae, Alessandro C. de Araùjo, Paulo Artaxo, Florian Ditas, Wolfgang Elbert, Jan-David Förster, Marco Aurélio Franco, Isabella Hrabe de Angelis, Jürgen Kesselmeier, Thomas Klimach, Leslie Ann Kremper, Eckhard Thines, David Walter, Jens Weber, Bettina Weber, Bernhard M. Fuchs, Ulrich Pöschl, and Christopher Pöhlker
Biogeosciences, 18, 4873–4887, https://doi.org/10.5194/bg-18-4873-2021, https://doi.org/10.5194/bg-18-4873-2021, 2021
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Bioaerosols in the atmosphere over the Amazon rain forest were analyzed by molecular biological staining and microscopy. Eukaryotic, bacterial, and archaeal aerosols were quantified in time series and altitude profiles which exhibited clear differences in number concentrations and vertical distributions. Our results provide insights into the sources and dispersion of different Amazonian bioaerosol types as a basis for a better understanding of biosphere–atmosphere interactions.
James Weber, Scott Archer-Nicholls, Nathan Luke Abraham, Youngsub M. Shin, Thomas J. Bannan, Carl J. Percival, Asan Bacak, Paulo Artaxo, Michael Jenkin, M. Anwar H. Khan, Dudley E. Shallcross, Rebecca H. Schwantes, Jonathan Williams, and Alex T. Archibald
Geosci. Model Dev., 14, 5239–5268, https://doi.org/10.5194/gmd-14-5239-2021, https://doi.org/10.5194/gmd-14-5239-2021, 2021
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The new mechanism CRI-Strat 2 features state-of-the-art isoprene chemistry not previously available in UKCA and improves UKCA's ability to reproduce observed concentrations of isoprene, monoterpenes, and OH in tropical regions. The enhanced ability to model isoprene, the most widely emitted non-methane volatile organic compound (VOC), will allow understanding of how isoprene and other biogenic VOCs affect atmospheric composition and, through biosphere–atmosphere feedbacks, climate change.
Jean-Daniel Paris, Aurélie Riandet, Efstratios Bourtsoukidis, Marc Delmotte, Antoine Berchet, Jonathan Williams, Lisa Ernle, Ivan Tadic, Hartwig Harder, and Jos Lelieveld
Atmos. Chem. Phys., 21, 12443–12462, https://doi.org/10.5194/acp-21-12443-2021, https://doi.org/10.5194/acp-21-12443-2021, 2021
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We measured atmospheric methane and CO2 by ship in the Middle East. We probe the origin of methane with a combination of light alkane measurements and modeling. We find strong influence from nearby oil and gas production over the Arabian Gulf. Comparing our data to inventories indicates that inventories overestimate sources from the upstream gas industry but underestimate emissions from oil extraction and processing. The Red Sea was under a complex mixture of sources due to human activity.
Patrick Dewald, Raphael Dörich, Jan Schuladen, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 14, 5501–5519, https://doi.org/10.5194/amt-14-5501-2021, https://doi.org/10.5194/amt-14-5501-2021, 2021
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Organic nitrates generated from the reaction between isoprene and the nitrate radical (ISOP-NITs) were detected via their thermal dissociation in heated quartz inlets to nitrogen dioxide monitored by cavity ring-down spectroscopy. The temperature-dependent dissociation profiles of ISOP-NITs in the presence of ozone (O3) are broad in contrast to narrow profiles of common reference compounds. We demonstrate that this broadening is caused by O3-assisted reactions of ISOP-NITs on quartz surfaces.
Raphael Dörich, Philipp Eger, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 14, 5319–5332, https://doi.org/10.5194/amt-14-5319-2021, https://doi.org/10.5194/amt-14-5319-2021, 2021
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We demonstrate in laboratory experiments that the formation of IOx anions (formed in reactions of I− with O3) or acetate anions (formed e.g. by the reaction of I− with peracetic acid) results in unexpected sensitivity of an iodide chemical ionisation mass spectrometer (I-CIMS) to HNO3 at a mass-to-charge ratio of 62. This helps explain observations of apparent high daytime levels of N2O5. Airborne measurements using I-CIMS confirm these conclusions.
Vinod Kumar, Julia Remmers, Steffen Beirle, Joachim Fallmann, Astrid Kerkweg, Jos Lelieveld, Mariano Mertens, Andrea Pozzer, Benedikt Steil, Marc Barra, Holger Tost, and Thomas Wagner
Atmos. Meas. Tech., 14, 5241–5269, https://doi.org/10.5194/amt-14-5241-2021, https://doi.org/10.5194/amt-14-5241-2021, 2021
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We present high-resolution regional atmospheric chemistry model simulations focused around Germany. We highlight the importance of spatial resolution of the model itself as well as the input emissions inventory and short-scale temporal variability of emissions for simulations. We propose a consistent approach for evaluating the simulated vertical distribution of NO2 using MAX-DOAS measurements while also considering its spatial sensitivity volume and change in sensitivity within this volume.
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.
Ivan Tadic, Clara M. Nussbaumer, Birger Bohn, Hartwig Harder, Daniel Marno, Monica Martinez, Florian Obersteiner, Uwe Parchatka, Andrea Pozzer, Roland Rohloff, Martin Zöger, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 8195–8211, https://doi.org/10.5194/acp-21-8195-2021, https://doi.org/10.5194/acp-21-8195-2021, 2021
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Although mechanisms of tropospheric ozone (O3) formation are well understood, studies reporting on ozone formation derived from field measurements are challenging and remain sparse in number. We use airborne measurements to quantify nitric oxide (NO) and O3 distributions in the upper troposphere over the Atlantic Ocean and western Africa and compare our measurements to model simulations. Our results show that NO and ozone formation are greatest over the tropical areas of western Africa.
Clara M. Nussbaumer, Ivan Tadic, Dirk Dienhart, Nijing Wang, Achim Edtbauer, Lisa Ernle, Jonathan Williams, Florian Obersteiner, Isidoro Gutiérrez-Álvarez, Hartwig Harder, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 7933–7945, https://doi.org/10.5194/acp-21-7933-2021, https://doi.org/10.5194/acp-21-7933-2021, 2021
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Lightning over continental and coastal areas is frequent and accompanied by deep convection, while lightning over marine areas and particularly in tropical cyclones is rare. This research presents in situ observations of the tropical storm Florence 2018 near Cabo Verde. We show the absence of lightning in the tropical storm despite the occurrence of deep convective processes by atmospheric trace gas measurements of O3, NO, CO, H2O2, DMS and CH2I.
Nils Friedrich, Philipp Eger, Justin Shenolikar, Nicolas Sobanski, Jan Schuladen, Dirk Dienhart, Bettina Hottmann, Ivan Tadic, Horst Fischer, Monica Martinez, Roland Rohloff, Sebastian Tauer, Hartwig Harder, Eva Y. Pfannerstill, Nijing Wang, Jonathan Williams, James Brooks, Frank Drewnick, Hang Su, Guo Li, Yafang Cheng, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 21, 7473–7498, https://doi.org/10.5194/acp-21-7473-2021, https://doi.org/10.5194/acp-21-7473-2021, 2021
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This paper uses NOx and NOz measurements from the 2017 AQABA ship campaign in the Mediterranean Sea and around the Arabian Peninsula to examine the influence e.g. of emissions from shipping and oil and gas production. Night-time losses of NOx dominated in the Arabian Gulf and in the Red Sea, whereas daytime losses were more important in the Mediterranean Sea. Nitric acid and organic nitrates were the most prevalent components of NOz.
Eva Y. Pfannerstill, Nina G. Reijrink, Achim Edtbauer, Akima Ringsdorf, Nora Zannoni, Alessandro Araújo, Florian Ditas, Bruna A. Holanda, Marta O. Sá, Anywhere Tsokankunku, David Walter, Stefan Wolff, Jošt V. Lavrič, Christopher Pöhlker, Matthias Sörgel, and Jonathan Williams
Atmos. Chem. Phys., 21, 6231–6256, https://doi.org/10.5194/acp-21-6231-2021, https://doi.org/10.5194/acp-21-6231-2021, 2021
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Tropical forests are globally significant for atmospheric chemistry. However, the mixture of reactive organic gases emitted by these ecosystems is poorly understood. By comprehensive observations at an Amazon forest site, we show that oxygenated species were previously underestimated in their contribution to the tropical-forest reactant mix. Our results show rain and temperature effects and have implications for models and the understanding of ozone and particle formation above tropical forests.
Wenjie Wang, Jipeng Qi, Jun Zhou, Bin Yuan, Yuwen Peng, Sihang Wang, Suxia Yang, Jonathan Williams, Vinayak Sinha, and Min Shao
Atmos. Meas. Tech., 14, 2285–2298, https://doi.org/10.5194/amt-14-2285-2021, https://doi.org/10.5194/amt-14-2285-2021, 2021
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We designed a new reactor for measurements of OH reactivity (i.e., OH radical loss frequency) based on the comparative reactivity method under
high-NOx conditions, such as in cities. We performed a series of laboratory tests to evaluate the new reactor. The new reactor was used in the field and performed well in measuring OH reactivity in air influenced by upwind cities.
Einar Karu, Mengze Li, Lisa Ernle, Carl A. M. Brenninkmeijer, Jos Lelieveld, and Jonathan Williams
Atmos. Meas. Tech., 14, 1817–1831, https://doi.org/10.5194/amt-14-1817-2021, https://doi.org/10.5194/amt-14-1817-2021, 2021
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A gas measurement device was developed to measure trace gases (ppt level) in the air based on an atomic emission detector. It combines a cryogenic pre-concentrator (CryoTrap), a gas chromatograph (GC), and a new high-resolution atomic emission detector (AED). The CryoTrap–GC–AED instrumental setup, limits of detection, and elemental performance are presented and discussed. Two measurement case studies are reported: one in a Finnish boreal forest and the other based on an aircraft campaign.
Domenico Taraborrelli, David Cabrera-Perez, Sara Bacer, Sergey Gromov, Jos Lelieveld, Rolf Sander, and Andrea Pozzer
Atmos. Chem. Phys., 21, 2615–2636, https://doi.org/10.5194/acp-21-2615-2021, https://doi.org/10.5194/acp-21-2615-2021, 2021
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Atmospheric pollutants from anthropogenic activities and biomass burning are usually regarded as ozone precursors. Monocyclic aromatics are no exception. Calculations with a comprehensive atmospheric model are consistent with this view but only for air masses close to pollution source regions. However, the same model predicts that aromatics, when transported to remote areas, may effectively destroy ozone. This loss of tropospheric ozone rivals the one attributed to bromine.
Sara Bacer, Sylvia C. Sullivan, Odran Sourdeval, Holger Tost, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 21, 1485–1505, https://doi.org/10.5194/acp-21-1485-2021, https://doi.org/10.5194/acp-21-1485-2021, 2021
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We investigate the relative importance of the rates of both microphysical processes and unphysical correction terms that act as sources or sinks of ice crystals in cold clouds. By means of numerical simulations performed with a global chemistry–climate model, we assess the relevance of these rates at global and regional scales. This estimation is of fundamental importance to assign priority to the development of microphysics parameterizations and compare model output with observations.
Klaus Klingmüller, Vlassis A. Karydis, Sara Bacer, Georgiy L. Stenchikov, and Jos Lelieveld
Atmos. Chem. Phys., 20, 15285–15295, https://doi.org/10.5194/acp-20-15285-2020, https://doi.org/10.5194/acp-20-15285-2020, 2020
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Particulate air pollution cools the climate and partially masks the greenhouse warming by reflecting sunlight and enhancing the reflection by clouds. The intensity of this cooling depends on interactions between pollution and desert dust within the atmosphere. Our simulations with a global atmospheric chemistry-climate model indicate that these interactions significantly weaken the cooling.
Matias Berasategui, Damien Amedro, Luc Vereecken, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 13541–13555, https://doi.org/10.5194/acp-20-13541-2020, https://doi.org/10.5194/acp-20-13541-2020, 2020
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Peracetic acid is one of the most abundant organic peroxides in the atmosphere. We combine experiments and theory to show that peracetic acid reacts orders of magnitude more slowly with OH than presently accepted, which results in a significant extension of its atmospheric lifetime.
Nina Löbs, David Walter, Cybelli G. G. Barbosa, Sebastian Brill, Rodrigo P. Alves, Gabriela R. Cerqueira, Marta de Oliveira Sá, Alessandro C. de Araújo, Leonardo R. de Oliveira, Florian Ditas, Daniel Moran-Zuloaga, Ana Paula Pires Florentino, Stefan Wolff, Ricardo H. M. Godoi, Jürgen Kesselmeier, Sylvia Mota de Oliveira, Meinrat O. Andreae, Christopher Pöhlker, and Bettina Weber
Biogeosciences, 17, 5399–5416, https://doi.org/10.5194/bg-17-5399-2020, https://doi.org/10.5194/bg-17-5399-2020, 2020
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Cryptogamic organisms, such as bryophytes, lichens, and algae, cover major parts of vegetation in the Amazonian rain forest, but their relevance in biosphere–atmosphere exchange, climate processes, and nutrient cycling is largely unknown.
Over the duration of 2 years we measured their water content, temperature, and light conditions to get better insights into their physiological activity patterns and thus their potential impact on local, regional, and even global biogeochemical processes.
Bettina Hottmann, Sascha Hafermann, Laura Tomsche, Daniel Marno, Monica Martinez, Hartwig Harder, Andrea Pozzer, Marco Neumaier, Andreas Zahn, Birger Bohn, Greta Stratmann, Helmut Ziereis, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 20, 12655–12673, https://doi.org/10.5194/acp-20-12655-2020, https://doi.org/10.5194/acp-20-12655-2020, 2020
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During OMO we observed enhanced mixing ratios of hydroperoxides (ROOH) in the Asian monsoon anticyclone (AMA) relative to the background. The observed mixing ratios are higher than steady-state calculations and EMAC simulations, especially in the AMA, indicating atmospheric transport of ROOH. Uncertainties in the scavenging efficiencies likely cause deviations from EMAC. Longitudinal gradients indicate a pool of ROOH towards the center of the AMA associated with upwind convection over India.
Nils Friedrich, Ivan Tadic, Jan Schuladen, James Brooks, Eoghan Darbyshire, Frank Drewnick, Horst Fischer, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 13, 5739–5761, https://doi.org/10.5194/amt-13-5739-2020, https://doi.org/10.5194/amt-13-5739-2020, 2020
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We present a new instrument for the measurement of NOx and NOy based on a combination of the thermal dissociation of NOy to NOx and cavity ring-down spectroscopic detection of NO2. It features a denuder to separate the contributions of gas-phase and particulate nitrates to NOy. We provide a detailed characterization of the instrument and briefly outline results from first deployments.
Nijing Wang, Achim Edtbauer, Christof Stönner, Andrea Pozzer, Efstratios Bourtsoukidis, Lisa Ernle, Dirk Dienhart, Bettina Hottmann, Horst Fischer, Jan Schuladen, John N. Crowley, Jean-Daniel Paris, Jos Lelieveld, and Jonathan Williams
Atmos. Chem. Phys., 20, 10807–10829, https://doi.org/10.5194/acp-20-10807-2020, https://doi.org/10.5194/acp-20-10807-2020, 2020
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Carbonyl compounds were measured on a ship travelling around the Arabian Peninsula in summer 2017, crossing both highly polluted and extremely clean regions of the marine boundary layer. We investigated the sources and sinks of carbonyls. The results from a global model showed a significant model underestimation for acetaldehyde, a molecule that can influence regional air chemistry. By adding a diurnal oceanic source, the model estimation was highly improved.
Patrick Dewald, Jonathan M. Liebmann, Nils Friedrich, Justin Shenolikar, Jan Schuladen, Franz Rohrer, David Reimer, Ralf Tillmann, Anna Novelli, Changmin Cho, Kangming Xu, Rupert Holzinger, François Bernard, Li Zhou, Wahid Mellouki, Steven S. Brown, Hendrik Fuchs, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 10459–10475, https://doi.org/10.5194/acp-20-10459-2020, https://doi.org/10.5194/acp-20-10459-2020, 2020
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We present direct measurements of NO3 reactivity resulting from the oxidation of isoprene by NO3 during an intensive simulation chamber study. Measurements were in excellent agreement with values calculated from measured isoprene amounts and the rate coefficient for the reaction of NO3 with isoprene. Comparison of the measurement with NO3 reactivities from non-steady-state and model calculations suggests that isoprene-derived RO2 and HO2 radicals account to ~ 50 % of overall NO3 losses.
Dominik Stolzenburg, Mario Simon, Ananth Ranjithkumar, Andreas Kürten, Katrianne Lehtipalo, Hamish Gordon, Sebastian Ehrhart, Henning Finkenzeller, Lukas Pichelstorfer, Tuomo Nieminen, Xu-Cheng He, Sophia Brilke, Mao Xiao, António Amorim, Rima Baalbaki, Andrea Baccarini, Lisa Beck, Steffen Bräkling, Lucía Caudillo Murillo, Dexian Chen, Biwu Chu, Lubna Dada, António Dias, Josef Dommen, Jonathan Duplissy, Imad El Haddad, Lukas Fischer, Loic Gonzalez Carracedo, Martin Heinritzi, Changhyuk Kim, Theodore K. Koenig, Weimeng Kong, Houssni Lamkaddam, Chuan Ping Lee, Markus Leiminger, Zijun Li, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Tatjana Müller, Wei Nie, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Matti P. Rissanen, Birte Rörup, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Mingyi Wang, Yonghong Wang, Stefan K. Weber, Daniela Wimmer, Peter J. Wlasits, Yusheng Wu, Qing Ye, Marcel Zauner-Wieczorek, Urs Baltensperger, Kenneth S. Carslaw, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Armin Hansel, Markku Kulmala, Jos Lelieveld, Rainer Volkamer, Jasper Kirkby, and Paul M. Winkler
Atmos. Chem. Phys., 20, 7359–7372, https://doi.org/10.5194/acp-20-7359-2020, https://doi.org/10.5194/acp-20-7359-2020, 2020
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Sulfuric acid is a major atmospheric vapour for aerosol formation. If new particles grow fast enough, they can act as cloud droplet seeds or affect air quality. In a controlled laboratory set-up, we demonstrate that van der Waals forces enhance growth from sulfuric acid. We disentangle the effects of ammonia, ions and particle hydration, presenting a complete picture of sulfuric acid growth from molecular clusters onwards. In a climate model, we show its influence on the global aerosol budget.
Ivan Tadic, John N. Crowley, Dirk Dienhart, Philipp Eger, Hartwig Harder, Bettina Hottmann, Monica Martinez, Uwe Parchatka, Jean-Daniel Paris, Andrea Pozzer, Roland Rohloff, Jan Schuladen, Justin Shenolikar, Sebastian Tauer, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 20, 6769–6787, https://doi.org/10.5194/acp-20-6769-2020, https://doi.org/10.5194/acp-20-6769-2020, 2020
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We present shipborne observations of NO, NO2, O3, HCHO, OH, HO2, H2O and the actinic flux obtained in the marine boundary layer (MBL) around the Arabian Peninsula during the summer 2017 AQABA ship campaign. NOx (NO+NO2) and O3 observations clearly showed anthropogenic influence in the MBL around the Arabian Peninsula. The observations were also used to calculate net O3 production in the MBL around the Arabian Peninsula, which was greatest over the northern Red Sea, Oman Gulf and Arabian Gulf.
Daniel Marno, Cheryl Ernest, Korbinian Hens, Umar Javed, Thomas Klimach, Monica Martinez, Markus Rudolf, Jos Lelieveld, and Hartwig Harder
Atmos. Meas. Tech., 13, 2711–2731, https://doi.org/10.5194/amt-13-2711-2020, https://doi.org/10.5194/amt-13-2711-2020, 2020
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In this study, a calibration device for OH and HO2 instruments is characterized at pressures of 275 to 1000 mbar, allowing instrument pressure sensitivity to be quantified to an accuracy of 22 % (1σ). Computational fluid dynamic simulations supporting the understanding of interactions between generated HOx and the instrument inlet led to enhanced determination of factors affecting instrument sensitivity.
Achim Edtbauer, Christof Stönner, Eva Y. Pfannerstill, Matias Berasategui, David Walter, John N. Crowley, Jos Lelieveld, and Jonathan Williams
Atmos. Chem. Phys., 20, 6081–6094, https://doi.org/10.5194/acp-20-6081-2020, https://doi.org/10.5194/acp-20-6081-2020, 2020
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Marine regions where deep nutrient-rich water is pushed towards the surface are called upwelling regions. In these nutrient-rich waters large algal blooms form which are the basis of the marine food web. We measured methane sulfonamide, a molecule containing sulfur and nitrogen, for the first time in ambient air and could show that the origin of this emission is an algal bloom near the Somalia upwelling. Sulfur-containing compounds from algae can promote particle formation over the oceans.
Peter H. Zimmermann, Carl A. M. Brenninkmeijer, Andrea Pozzer, Patrick Jöckel, Franziska Winterstein, Andreas Zahn, Sander Houweling, and Jos Lelieveld
Atmos. Chem. Phys., 20, 5787–5809, https://doi.org/10.5194/acp-20-5787-2020, https://doi.org/10.5194/acp-20-5787-2020, 2020
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The atmospheric abundance of the greenhouse gas methane is determined by interacting emission sources and sinks in a dynamic global environment. In this study, its global budget from 1997 to 2016 is simulated with a general circulation model using emission estimates of 11 source categories. The model results are evaluated against 17 ground station and 320 intercontinental flight observation series. Deviations are used to re-scale the emission quantities with the aim of matching observations.
Philipp G. Eger, Jan Schuladen, Nicolas Sobanski, Horst Fischer, Einar Karu, Jonathan Williams, Matthieu Riva, Qiaozhi Zha, Mikael Ehn, Lauriane L. J. Quéléver, Simon Schallhart, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 3697–3711, https://doi.org/10.5194/acp-20-3697-2020, https://doi.org/10.5194/acp-20-3697-2020, 2020
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Pyruvic acid, CH3C(O)C(O)OH, is an organic acid of biogenic origin that plays a crucial role in plant metabolism, is present in tropospheric air in both gas-phase and aerosol-phase, and is implicated in the formation of secondary organic aerosols. From the first gas-phase measurements of pyruvic acid in the Finnish boreal forest in September 2016 we derive its source strength and discuss potential sources and sinks, with a focus on the relevance of gas-phase pyruvic acid for radical chemistry.
Matthew Forrest, Holger Tost, Jos Lelieveld, and Thomas Hickler
Geosci. Model Dev., 13, 1285–1309, https://doi.org/10.5194/gmd-13-1285-2020, https://doi.org/10.5194/gmd-13-1285-2020, 2020
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We have integrated the LPJ-GUESS dynamic global vegetation model into the EMAC atmospheric chemistry-enabled GCM (general circulation model). This combined framework will enable the investigation of many land–atmosphere interactions and feedbacks with state-of-the-art simulation models. Initial results show that using the climate produced by EMAC together with LPJ-GUESS produces an acceptable representation of the global vegetation.
Matias Berasategui, Damien Amedro, Achim Edtbauer, Jonathan Williams, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 2695–2707, https://doi.org/10.5194/acp-20-2695-2020, https://doi.org/10.5194/acp-20-2695-2020, 2020
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We have determined the rate coefficient and mechanism for the reaction of the OH radical with methane sulphonamide, a trace gas which has recently been found in the atmosphere. The rate coefficient is 1.4 × 10−13 cm3 molec.−1 s−1, which indicates a tropospheric lifetime of > 2 months. The observation of CO, CO2, SO2, HNO3, HCOOH, and N2O products enabled us to derive a detailed reaction mechanism for the reaction, which proceeds predominantly by H abstraction from the CH3 group.
Ying Chen, Yafang Cheng, Nan Ma, Chao Wei, Liang Ran, Ralf Wolke, Johannes Größ, Qiaoqiao Wang, Andrea Pozzer, Hugo A. C. Denier van der Gon, Gerald Spindler, Jos Lelieveld, Ina Tegen, Hang Su, and Alfred Wiedensohler
Atmos. Chem. Phys., 20, 771–786, https://doi.org/10.5194/acp-20-771-2020, https://doi.org/10.5194/acp-20-771-2020, 2020
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Particulate nitrate is one of the most important climate cooling agents. Our results show that interaction with sea-salt aerosol can shift nitrate to larger sized particles (redistribution effect), weakening its direct cooling effect. The modelling results indicate strong redistribution over coastal and offshore regions worldwide as well as continental Europe. Improving the consideration of the redistribution effect in global models fosters a better understanding of climate change.
Nina Löbs, Cybelli G. G. Barbosa, Sebastian Brill, David Walter, Florian Ditas, Marta de Oliveira Sá, Alessandro C. de Araújo, Leonardo R. de Oliveira, Ricardo H. M. Godoi, Stefan Wolff, Meike Piepenbring, Jürgen Kesselmeier, Paulo Artaxo, Meinrat O. Andreae, Ulrich Pöschl, Christopher Pöhlker, and Bettina Weber
Atmos. Meas. Tech., 13, 153–164, https://doi.org/10.5194/amt-13-153-2020, https://doi.org/10.5194/amt-13-153-2020, 2020
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Bioaerosols are considered to play a relevant role in atmospheric processes, but their sources, properties, and spatiotemporal distribution in the atmosphere are not yet well characterized. Measurement data on the release of fungal spores under natural conditions are also sparse. Here, we present an experimental approach to analyze and quantify the spore release from fungi and other spore-producing organisms under natural and laboratory conditions.
Tanja J. Schuck, Ann-Katrin Blank, Elisa Rittmeier, Jonathan Williams, Carl A. M. Brenninkmeijer, Andreas Engel, and Andreas Zahn
Atmos. Meas. Tech., 13, 73–84, https://doi.org/10.5194/amt-13-73-2020, https://doi.org/10.5194/amt-13-73-2020, 2020
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Air sample collection aboard aircraft is a tool to measure atmospheric trace gas mixing ratios at altitude. We present results on the stability of 28 halocarbons during storage of air samples collected in stainless-steel flasks inside an automated air sampling unit which is part of the CARIBIC instrument package. Selected fluorinated compounds grew during the experiments while short-lived compounds were depleted. Individual substances were additionally influenced by high mixing ratios of ozone.
Boris Bonn, Ruth-Kristina Magh, Joseph Rombach, and Jürgen Kreuzwieser
Biogeosciences, 16, 4627–4645, https://doi.org/10.5194/bg-16-4627-2019, https://doi.org/10.5194/bg-16-4627-2019, 2019
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The effect of soil water availability (SWA) on emissions of isoprenoids by trees was studied by setting up a parameterization from published data. SWA impact on isoprene emissions can be described by a growth type curve, while monoterpene emissions display a pattern reflecting plants’ stomata opening. Sesquiterpene fluxes tend to increase at the start of severe drought until resources decline. Feedbacks on atmospheric processes such as ozone and aerosol particles are further studied.
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.
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.
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.
Klaus Klingmüller, Jos Lelieveld, Vlassis A. Karydis, and Georgiy L. Stenchikov
Atmos. Chem. Phys., 19, 7397–7408, https://doi.org/10.5194/acp-19-7397-2019, https://doi.org/10.5194/acp-19-7397-2019, 2019
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Within the atmosphere, desert dust and anthropogenic pollution are mixed and interact, which affects the abundance and optical properties of the particulate matter. This results in an anthropogenic climate forcing associated with mineral dust notwithstanding the natural origin of most aeolian dust. With a global chemistry–climate model, we estimate this forcing to represent a considerable fraction of the total dust forcing.
Efstratios Bourtsoukidis, Lisa Ernle, John N. Crowley, Jos Lelieveld, Jean-Daniel Paris, Andrea Pozzer, David Walter, and Jonathan Williams
Atmos. Chem. Phys., 19, 7209–7232, https://doi.org/10.5194/acp-19-7209-2019, https://doi.org/10.5194/acp-19-7209-2019, 2019
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We report on results that demonstrate the utility of non-methane hydrocarbons as source/sink identification tracers while providing their mixing ratios around the Arabian Peninsula. By introducing novel data-analysis approaches, we establish a new method for separating associated and non-associated (with liquids) gases. We formulate a relationship between hydrocarbon oxidative pairs that can be used to evaluate the relative abundance of the hydroxyl and chlorine radicals in the troposphere.
Ralph Dlugi, Martina Berger, Chinmay Mallik, Anywhere Tsokankunku, Michael Zelger, Otávio C. Acevedo, Efstratios Bourtsoukidis, Andreas Hofzumahaus, Jürgen Kesselmeier, Gerhard Kramm, Daniel Marno, Monica Martinez, Anke C. Nölscher, Huug Ouwersloot, Eva Y. Pfannerstill, Franz Rohrer, Sebastian Tauer, Jonathan Williams, Ana-Maria Yáñez-Serrano, Meinrat O. Andreae, Hartwig Harder, and Matthias Sörgel
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-1325, https://doi.org/10.5194/acp-2018-1325, 2019
Publication in ACP not foreseen
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Incomplete mixing (segregation) results in reduced chemical reaction rates compared to those expected from mean values and rate constants. Segregation has been suggested to cause discrepancies between modelled and measured OH radical concentrations. In this work, we summarize the intensities of segregation for the reaction of OH and isoprene for different field and modelling studies and compare those to our results from measurements in a pristine environment.
Meryem Tanarhte, Sara Bacer, Susannah M. Burrows, J. Alex Huffman, Kyle M. Pierce, Andrea Pozzer, Roland Sarda-Estève, Nicole J. Savage, and Jos Lelieveld
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2019-251, https://doi.org/10.5194/acp-2019-251, 2019
Publication in ACP not foreseen
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Bioaerosols have been an important topic in atmospheric science in the last two decades. This paper compares different emission parametrizations used in fungal spores modeling and compare their results to two sets of new observational datasets. It emphasises their uncertainties in order to improve their modeling in the future. This comparison is addressed primarily to the scientific community (publishing in ACP) interested in this type of modeling and the related experimental work in this field.
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.
Thomas Behrendt, Elisa C. P. Catão, Rüdiger Bunk, Zhigang Yi, Elena Schweer, Steffen Kolb, Jürgen Kesselmeier, and Susan Trumbore
SOIL, 5, 121–135, https://doi.org/10.5194/soil-5-121-2019, https://doi.org/10.5194/soil-5-121-2019, 2019
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We measured net fluxes of OCS from nine soils with different land use in a dynamic chamber system and analyzed for one soil RNA relative abundance and gene transcripts. Our data suggest that indeed carbonic anhydrase (CA) plays an important role for OCS exchange, but the role of other enzymes might have been underestimated. Our study is the first assessment of the environmental significance of different microbial groups producing and consuming OCS by various enzymes other than CA.
Guo Li, Yafang Cheng, Uwe Kuhn, Rongjuan Xu, Yudong Yang, Hannah Meusel, Zhibin Wang, Nan Ma, Yusheng Wu, Meng Li, Jonathan Williams, Thorsten Hoffmann, Markus Ammann, Ulrich Pöschl, Min Shao, and Hang Su
Atmos. Chem. Phys., 19, 2209–2232, https://doi.org/10.5194/acp-19-2209-2019, https://doi.org/10.5194/acp-19-2209-2019, 2019
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VOCs play a key role in atmospheric chemistry. Emission and deposition on soil have been suggested as important sources and sinks of atmospheric trace gases. The exchange characteristics and heterogeneous chemistry of VOCs on soil, however, are not well understood. We used a newly designed differential coated-wall flow tube system to investigate the long-term variability of bidirectional air–soil exchange of 13 VOCs at ambient air conditions of an urban background site in Beijing.
Laura Tomsche, Andrea Pozzer, Narendra Ojha, Uwe Parchatka, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 19, 1915–1939, https://doi.org/10.5194/acp-19-1915-2019, https://doi.org/10.5194/acp-19-1915-2019, 2019
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The Asian monsoon anticyclone (AMA) is an annual phenomenon in the northern hemispheric upper troposphere (UT) and lower stratosphere. We performed in situ measurements of carbon monoxide (CO) and methane (CH4) in the monsoon outflow region and in background air in the UT (Mediterranean, Arabian Peninsula, Arabian Sea) using airborne optical absorption spectroscopy during the Oxidation Mechanism Observations mission (summer 2015). The trace gases increased within the AMA, particularly CH4.
Yingying Yan, David Cabrera-Perez, Jintai Lin, Andrea Pozzer, Lu Hu, Dylan B. Millet, William C. Porter, and Jos Lelieveld
Geosci. Model Dev., 12, 111–130, https://doi.org/10.5194/gmd-12-111-2019, https://doi.org/10.5194/gmd-12-111-2019, 2019
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The GEOS-Chem model has been updated with the SAPRC-11 aromatics chemical mechanism to evaluate global and regional effects of aromatics on tropospheric oxidation capacity. Our results reveal relatively slight changes in ozone, hydroxyl radical, and nitrogen oxides on a global mean basis (1–4 %), although remarkable regional differences (5–20 %) exist near the source regions. Improved representation of aromatics is important to simulate the tropospheric oxidation.
Sebastian Ehrhart, Eimear M. Dunne, Hanna E. Manninen, Tuomo Nieminen, Jos Lelieveld, and Andrea Pozzer
Geosci. Model Dev., 11, 4987–5001, https://doi.org/10.5194/gmd-11-4987-2018, https://doi.org/10.5194/gmd-11-4987-2018, 2018
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.
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.
Mira L. Pöhlker, Florian Ditas, Jorge Saturno, Thomas Klimach, Isabella Hrabě de Angelis, Alessandro C. Araùjo, Joel Brito, Samara Carbone, Yafang Cheng, Xuguang Chi, Reiner Ditz, Sachin S. Gunthe, Bruna A. Holanda, Konrad Kandler, Jürgen Kesselmeier, Tobias Könemann, Ovid O. Krüger, Jošt V. Lavrič, Scot T. Martin, Eugene Mikhailov, Daniel Moran-Zuloaga, Luciana V. Rizzo, Diana Rose, Hang Su, Ryan Thalman, David Walter, Jian Wang, Stefan Wolff, Henrique M. J. Barbosa, Paulo Artaxo, Meinrat O. Andreae, Ulrich Pöschl, and Christopher Pöhlker
Atmos. Chem. Phys., 18, 10289–10331, https://doi.org/10.5194/acp-18-10289-2018, https://doi.org/10.5194/acp-18-10289-2018, 2018
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This paper presents the aerosol and cloud condensation nuclei (CCN) variability for characteristic atmospheric states – such as biomass burning, long-range transport, and pristine rain forest conditions – in the vulnerable and climate-relevant Amazon Basin. It summarizes the key properties of aerosol and CCN and, thus, provides a basis for an in-depth analysis of aerosol–cloud interactions in the Amazon region.
Erika von Schneidemesser, Boris Bonn, Tim M. Butler, Christian Ehlers, Holger Gerwig, Hannele Hakola, Heidi Hellén, Andreas Kerschbaumer, Dieter Klemp, Claudia Kofahl, Jürgen Kura, Anja Lüdecke, Rainer Nothard, Axel Pietsch, Jörn Quedenau, Klaus Schäfer, James J. Schauer, Ashish Singh, Ana-Maria Villalobos, Matthias Wiegner, and Mark G. Lawrence
Atmos. Chem. Phys., 18, 8621–8645, https://doi.org/10.5194/acp-18-8621-2018, https://doi.org/10.5194/acp-18-8621-2018, 2018
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This paper provides an overview of the measurements done at an urban background site in Berlin from June-August of 2014. Results show that natural source contributions to ozone and particulate matter (PM) air pollutants are substantial. Large contributions of secondary aerosols formed in the atmosphere to PM10 concentrations were quantified. An analysis of the sources also identified contributions to PM from plant-based sources, vehicles, and a small contribution from wood burning.
Aristeidis K. Georgoulias, Athanasios Tsikerdekis, Vassilis Amiridis, Eleni Marinou, Angela Benedetti, Prodromos Zanis, Georgia Alexandri, Lucia Mona, Konstantinos A. Kourtidis, and Jos Lelieveld
Atmos. Chem. Phys., 18, 8601–8620, https://doi.org/10.5194/acp-18-8601-2018, https://doi.org/10.5194/acp-18-8601-2018, 2018
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In this work, the MACC reanalysis dust product is evaluated over Europe, Northern Africa and the Middle East using the EARLINET-optimized CALIOP/CALIPSO pure dust satellite-based product LIVAS (2007–2012). As dust plays a determinant role in processes related to weather and climate, human healt, and the economy, it is obvious that adequately simulating the amount of dust and its optical properties is essential. Our results could be used as a reference in future climate model evaluations.
Meryem Tanarhte, Sara Bacer, Susannah M. Burrows, J. Alex Huffman, Kyle M. Pierce, Andrea Pozzer, Roland Sarda-Estève, Nicole J. Savage, and Jos Lelieveld
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-361, https://doi.org/10.5194/acp-2018-361, 2018
Revised manuscript not accepted
Yingying Yan, Andrea Pozzer, Narendra Ojha, Jintai Lin, and Jos Lelieveld
Atmos. Chem. Phys., 18, 5589–5605, https://doi.org/10.5194/acp-18-5589-2018, https://doi.org/10.5194/acp-18-5589-2018, 2018
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Surface-based measurements from the EMEP network and EMAC model simulations are used to estimate the European surface ozone changes over 1995–2014. It shows a significantly decreasing trend in the 95th percentile ozone concentrations, while increasing in the 5th percentile ozone. Sensitivity simulations and statistical analysis show that a decrease in European anthropogenic emissions had contrasting effects on surface ozone trends between the 95th and 5th percentile levels.
Klaus Klingmüller, Swen Metzger, Mohamed Abdelkader, Vlassis A. Karydis, Georgiy L. Stenchikov, Andrea Pozzer, and Jos Lelieveld
Geosci. Model Dev., 11, 989–1008, https://doi.org/10.5194/gmd-11-989-2018, https://doi.org/10.5194/gmd-11-989-2018, 2018
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More than 1 billion tons of mineral dust particles are raised into the atmosphere every year, which has a significant impact on climate, society and ecosystems. The location, time and amount of dust emissions depend on surface and wind conditions. In the atmospheric chemistry–climate model EMAC, we have updated the relevant surface data and equations. Our validation shows that the updates substantially improve the agreement of model results and observations.
Jonathan Liebmann, Einar Karu, Nicolas Sobanski, Jan Schuladen, Mikael Ehn, Simon Schallhart, Lauriane Quéléver, Heidi Hellen, Hannele Hakola, Thorsten Hoffmann, Jonathan Williams, Horst Fischer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 18, 3799–3815, https://doi.org/10.5194/acp-18-3799-2018, https://doi.org/10.5194/acp-18-3799-2018, 2018
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Using a newly developed experimental setup, we have made the first direct measurements (during autumn 2016) of NO3 reactivity in the Finnish boreal forest. The NO3 reactivity was generally very high (maximum value of 0.94/s) so that daytime reaction with organics was a substantial fraction of the NO3 loss. Observations of biogenic hydrocarbons (BVOCs) suggested a dominant role for monoterpenes in determining the NO3 reactivity, which displayed a strong vertical gradient between 8.5 and 25 m.
Ana María Yáñez-Serrano, Anke Christine Nölscher, Efstratios Bourtsoukidis, Eliane Gomes Alves, Laurens Ganzeveld, Boris Bonn, Stefan Wolff, Marta Sa, Marcia Yamasoe, Jonathan Williams, Meinrat O. Andreae, and Jürgen Kesselmeier
Atmos. Chem. Phys., 18, 3403–3418, https://doi.org/10.5194/acp-18-3403-2018, https://doi.org/10.5194/acp-18-3403-2018, 2018
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This study shows the measurements of concentration of different monoterpene species in terms of height, time of day and season. Speciation seems similar during the dry seasons but changes with season. Furthermore, reactivity with the different oxidants demonstrated that a higher abundance of a monoterpene species does not automatically imply higher reactivity and that the most abundant monoterpene may not be the most atmospheric chemically relevant compound.
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.
Rüdiger Bunk, Zhigang Yi, Thomas Behrendt, Dianming Wu, Meinrat Otto Andreae, and Jürgen Kesselmeier
Biogeosciences Discuss., https://doi.org/10.5194/bg-2018-20, https://doi.org/10.5194/bg-2018-20, 2018
Manuscript not accepted for further review
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We examined the OCS exchange of four soils with the atmosphere. The laboratory setup used allowed to monitor this exchange while simultaneously monitor soil moisture. The OCS exchange of those soils was measured over full range from very wet to very dry.
We found that uptake of OCS is highly dependent on soil moisture, that probably heterotroph and autotrophs drive the uptake at different soil moistures and that the role of soils as net consumer or producers of OCS may vary with soil moisture.
Hannah Meusel, Alexandra Tamm, Uwe Kuhn, Dianming Wu, Anna Lena Leifke, Sabine Fiedler, Nina Ruckteschler, Petya Yordanova, Naama Lang-Yona, Mira Pöhlker, Jos Lelieveld, Thorsten Hoffmann, Ulrich Pöschl, Hang Su, Bettina Weber, and Yafang Cheng
Atmos. Chem. Phys., 18, 799–813, https://doi.org/10.5194/acp-18-799-2018, https://doi.org/10.5194/acp-18-799-2018, 2018
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The photolysis of nitrous acid (HONO) forms the OH radical. However, not all sources are known. Recent studies showed that HONO can be emitted from soil but they did not evaluate the importance to the HONO budget. In this work HONO emissions from 43 soil and biological soil crust samples from Cyprus were measured in a dynamic chamber and extrapolated to the real atmosphere. A large fraction of the local missing source (published earlier; Meusel et al., 2016) could be assigned to soil emissions.
Efstratios Bourtsoukidis, Frank Helleis, Laura Tomsche, Horst Fischer, Rolf Hofmann, Jos Lelieveld, and Jonathan Williams
Atmos. Meas. Tech., 10, 5089–5105, https://doi.org/10.5194/amt-10-5089-2017, https://doi.org/10.5194/amt-10-5089-2017, 2017
Amit Sharma, Narendra Ojha, Andrea Pozzer, Kathleen A. Mar, Gufran Beig, Jos Lelieveld, and Sachin S. Gunthe
Atmos. Chem. Phys., 17, 14393–14413, https://doi.org/10.5194/acp-17-14393-2017, https://doi.org/10.5194/acp-17-14393-2017, 2017
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We evaluate the numerical simulations of surface ozone during pre-monsoon season against a network of stations including clean, rural and polluted urban environments in the south Asian region. Significant effects of the employed emission inventory and chemical mechanism on the simulated ozone are found during the noon hours of intense photochemistry. The presented evaluation on the diurnal timescale would have implications for assessing ozone buildup and impacts on human health and crop yields.
Andrea Pozzer, Alexandra P. Tsimpidi, Vlassis A. Karydis, Alexander de Meij, and Jos Lelieveld
Atmos. Chem. Phys., 17, 12813–12826, https://doi.org/10.5194/acp-17-12813-2017, https://doi.org/10.5194/acp-17-12813-2017, 2017
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This study shows that agricultural emissions are important for air quality and their reduction can effectively reduce the concentration of fine particles and their associated premature mortality. Therefore, emission control policies, especially in North America and Europe, should also involve strong ammonia emission decreases to optimally reduce fine-particle concentration.
Hendrik Fuchs, Anna Novelli, Michael Rolletter, Andreas Hofzumahaus, Eva Y. Pfannerstill, Stephan Kessel, Achim Edtbauer, Jonathan Williams, Vincent Michoud, Sebastien Dusanter, Nadine Locoge, Nora Zannoni, Valerie Gros, Francois Truong, Roland Sarda-Esteve, Danny R. Cryer, Charlotte A. Brumby, Lisa K. Whalley, Daniel Stone, Paul W. Seakins, Dwayne E. Heard, Coralie Schoemaecker, Marion Blocquet, Sebastien Coudert, Sebastien Batut, Christa Fittschen, Alexander B. Thames, William H. Brune, Cheryl Ernest, Hartwig Harder, Jennifer B. A. Muller, Thomas Elste, Dagmar Kubistin, Stefanie Andres, Birger Bohn, Thorsten Hohaus, Frank Holland, Xin Li, Franz Rohrer, Astrid Kiendler-Scharr, Ralf Tillmann, Robert Wegener, Zhujun Yu, Qi Zou, and Andreas Wahner
Atmos. Meas. Tech., 10, 4023–4053, https://doi.org/10.5194/amt-10-4023-2017, https://doi.org/10.5194/amt-10-4023-2017, 2017
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Hydroxyl radical reactivity (k(OH)) is closely related to processes that lead to the formation of oxidised, secondary pollutants such as ozone and aerosol. In order to compare the performances of instruments measuring k(OH), experiments were conducted in the simulation chamber SAPHIR. Chemical conditions were chosen either to be representative of the atmosphere or to test potential limitations of instruments. Overall, the results show that instruments are capable of measuring k(OH).
David Cabrera-Perez, Domenico Taraborrelli, Jos Lelieveld, Thorsten Hoffmann, and Andrea Pozzer
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2017-928, https://doi.org/10.5194/acp-2017-928, 2017
Revised manuscript not accepted
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Aromatic compounds are present in rural and urban atmospheres. The aim of this work is to disentangle the impacts of these compounds in different important atmospheric chemical species with the help of a numerical model. Aromatics have low impact OH, NOx and Ozone concentrations in the global scale (below 4 %). The impact however is larger in the regional scale (up to 10 %). The largest impact is in glyoxal and NO3 concentrations, with changes up to 10 % globally and 40 % regionally.
Heiko Bozem, Andrea Pozzer, Hartwig Harder, Monica Martinez, Jonathan Williams, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 17, 11835–11848, https://doi.org/10.5194/acp-17-11835-2017, https://doi.org/10.5194/acp-17-11835-2017, 2017
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We present a case study of deep convection over Germany in July 2007 within the framework of the HOOVER II project. Airborne in situ measurements within the in- and outflow regions of an isolated thunderstorm provide a unique data set to study the influence of deep convection on the transport efficiency of soluble and insoluble trace gases. Despite their high solubility HCHO and H2O2 show enhanced concentrations in the outflow presumably due to degassing from cloud droplets during freezing.
Hannah Meusel, Yasin Elshorbany, Uwe Kuhn, Thorsten Bartels-Rausch, Kathrin Reinmuth-Selzle, Christopher J. Kampf, Guo Li, Xiaoxiang Wang, Jos Lelieveld, Ulrich Pöschl, Thorsten Hoffmann, Hang Su, Markus Ammann, and Yafang Cheng
Atmos. Chem. Phys., 17, 11819–11833, https://doi.org/10.5194/acp-17-11819-2017, https://doi.org/10.5194/acp-17-11819-2017, 2017
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In this study we investigated protein nitration and decomposition by light in the presence of NO2 via flow tube measurements. Nitrated proteins have an enhanced allergenic potential but so far nitration was only studied in dark conditions. Under irradiated conditions we found that proteins predominantly decompose while forming nitrous acid (HONO) an important precursor of the OH radical. Unlike other studies on heterogeneous NO2 conversion we found a stable HONO formation over a long period.
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.
Alexander Geiß, Matthias Wiegner, Boris Bonn, Klaus Schäfer, Renate Forkel, Erika von Schneidemesser, Christoph Münkel, Ka Lok Chan, and Rainer Nothard
Atmos. Meas. Tech., 10, 2969–2988, https://doi.org/10.5194/amt-10-2969-2017, https://doi.org/10.5194/amt-10-2969-2017, 2017
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Based on measurements with a ceilometer and from an air quality network, the relationship between the mixing layer height (MLH) and near surface concentrations of pollutants was investigated for summer 2014 in Berlin. It was found that the heterogeneity of the concentrations exceeds the differences due to different MLH retrievals. In particular for PM10 it seems to be unrealistic to find correlations between MLH and concentrations representative for an entire metropolitan area in flat terrain.
Bettina Derstroff, Imke Hüser, Efstratios Bourtsoukidis, John N. Crowley, Horst Fischer, Sergey Gromov, Hartwig Harder, Ruud H. H. Janssen, Jürgen Kesselmeier, Jos Lelieveld, Chinmay Mallik, Monica Martinez, Anna Novelli, Uwe Parchatka, Gavin J. Phillips, Rolf Sander, Carina Sauvage, Jan Schuladen, Christof Stönner, Laura Tomsche, and Jonathan Williams
Atmos. Chem. Phys., 17, 9547–9566, https://doi.org/10.5194/acp-17-9547-2017, https://doi.org/10.5194/acp-17-9547-2017, 2017
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The aim of the study was to examine aged air masses being transported from the European continent towards Cyprus. Longer-lived oxygenated volatile organic compounds (OVOCs) such as methanol were mainly impacted by long-distance transport and showed higher values in air masses from eastern Europe than in a flow regime from the west. The impact of the transport through the marine boundary layer as well as the influence of the residual layer/free troposphere on OVOCs were studied.
Stephan Keßel, David Cabrera-Perez, Abraham Horowitz, Patrick R. Veres, Rolf Sander, Domenico Taraborrelli, Maria Tucceri, John N. Crowley, Andrea Pozzer, Christof Stönner, Luc Vereecken, Jos Lelieveld, and Jonathan Williams
Atmos. Chem. Phys., 17, 8789–8804, https://doi.org/10.5194/acp-17-8789-2017, https://doi.org/10.5194/acp-17-8789-2017, 2017
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In this study we identify an often overlooked stable oxide of carbon, namely carbon suboxide (C3O2), in ambient air. We have made C3O2 and in the laboratory determined its absorption cross section data and the rate of reaction with two important atmospheric oxidants, OH and O3. By incorporating known sources and sinks in a global model we have generated a first global picture of the distribution of this species in the atmosphere.
Anna Novelli, Korbinian Hens, Cheryl Tatum Ernest, Monica Martinez, Anke C. Nölscher, Vinayak Sinha, Pauli Paasonen, Tuukka Petäjä, Mikko Sipilä, Thomas Elste, Christian Plass-Dülmer, Gavin J. Phillips, Dagmar Kubistin, Jonathan Williams, Luc Vereecken, Jos Lelieveld, and Hartwig Harder
Atmos. Chem. Phys., 17, 7807–7826, https://doi.org/10.5194/acp-17-7807-2017, https://doi.org/10.5194/acp-17-7807-2017, 2017
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The ambient concentration of stabilised Criegee intermediates (SCIs) was estimated for two
environments using field data. The low concentrations predicted indicate that SCIs are
unlikely to have a large impact on atmospheric chemistry. Concurrent measurements of an OH background signal using the Mainz IPI-LIF-FAGE instrument were found to be consistent with the chemistry of SCIs during the measurement campaigns.
Alexandra P. Tsimpidi, Vlassis A. Karydis, Spyros N. Pandis, and Jos Lelieveld
Atmos. Chem. Phys., 17, 7345–7364, https://doi.org/10.5194/acp-17-7345-2017, https://doi.org/10.5194/acp-17-7345-2017, 2017
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We analyzed the sensitivity of model-predicted global-scale OA to parameters and assumptions that control primary emissions, photochemical aging, and the scavenging efficiency of LVOCs, SVOCs, and IVOCs. The simulated OA concentrations were evaluated against a global dataset of AMS measurements. According to our analysis, a combination of increased IVOCs and decreased hygroscopicity of the freshly emitted IVOCs can help reduce discrepancies between simulated SOA and observed OOA concentrations.
Yudong Yang, Min Shao, Stephan Keßel, Yue Li, Keding Lu, Sihua Lu, Jonathan Williams, Yuanhang Zhang, Liming Zeng, Anke C. Nölscher, Yusheng Wu, Xuemei Wang, and Junyu Zheng
Atmos. Chem. Phys., 17, 7127–7142, https://doi.org/10.5194/acp-17-7127-2017, https://doi.org/10.5194/acp-17-7127-2017, 2017
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Total OH reactivity is an important parameter to evaluate understanding of atmospheric chemistry, especially the VOC contribution to air pollution. Measured by comparative reactivity methods, total OH reactivity in Beijing and Heshan revealed significant differences between measured and calculated results, such as missing reactivity, which were related to unmeasured primary or secondary species. This missing reactivity would introduce a 21–30 % underestimation for ozone production efficiency.
Narendra Ojha, Andrea Pozzer, Dimitris Akritidis, and Jos Lelieveld
Atmos. Chem. Phys., 17, 6743–6757, https://doi.org/10.5194/acp-17-6743-2017, https://doi.org/10.5194/acp-17-6743-2017, 2017
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We investigate the processes, frequency of occurrence and seasonality, and effects of strongly enhanced ozone layers in the middle–upper troposphere (SOPs) over the Himalayas using a global model (EMAC). Rapid transport of stratospheric air masses is found as a key underlying process. Model predicts more frequent SOP events during the pre-monsoon. SOPs are found to significantly enhance the tropospheric ozone column over the Himalayas.
Vlassis A. Karydis, Alexandra P. Tsimpidi, Sara Bacer, Andrea Pozzer, Athanasios Nenes, and Jos Lelieveld
Atmos. Chem. Phys., 17, 5601–5621, https://doi.org/10.5194/acp-17-5601-2017, https://doi.org/10.5194/acp-17-5601-2017, 2017
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The importance of mineral dust for cloud droplet formation is studied by considering the adsorption activation of insoluble dust particles and the thermodynamic interactions between mineral cations and inorganic anions. This study demonstrates that a comprehensive treatment of the CCN activity of mineral dust and its chemical and thermodynamic interactions with inorganic species by chemistry climate models is important to realistically account for aerosol–chemistry–cloud–climate interaction.
Jonathan M. Liebmann, Gerhard Schuster, Jan B. Schuladen, Nicolas Sobanski, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 10, 1241–1258, https://doi.org/10.5194/amt-10-1241-2017, https://doi.org/10.5194/amt-10-1241-2017, 2017
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We describe the first instrument for measurement of the rate constant for reactive loss (i.e. the total reactivity) of NO3 in ambient air. This is essentially a measureement of the lifetime of NO3 and will help assess the role of NO3 and N2O5 in conversion of reactive nitrogen oxides to reservoir species in the troposphere.
Nicolas Sobanski, Jim Thieser, Jan Schuladen, Carina Sauvage, Wei Song, Jonathan Williams, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 17, 4115–4130, https://doi.org/10.5194/acp-17-4115-2017, https://doi.org/10.5194/acp-17-4115-2017, 2017
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We investigated the formation of gas-phase organic nitrates at a forested semi-urban site. This work constitutes the first detailed analysis of the sum of organic nitrate mixing ratios measured by thermal dissociation cavity ring-down spectroscopy in continental Europe. Day (OH-initiated) and night-time (NO3-initiated) production of alkyl nitrates proceed at similar rates.
Mohamed Abdelkader, Swen Metzger, Benedikt Steil, Klaus Klingmüller, Holger Tost, Andrea Pozzer, Georgiy Stenchikov, Leonard Barrie, and Jos Lelieveld
Atmos. Chem. Phys., 17, 3799–3821, https://doi.org/10.5194/acp-17-3799-2017, https://doi.org/10.5194/acp-17-3799-2017, 2017
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We present a modeling study on the impacts of the key processes (dust emission flux, convection and dust aging parameterizations) that control the transatlantic dust transport using an advanced version of the EMAC atmospheric chemistry general circulation model. We define the
direct effect of dust agingas an increase in the AOD as a result of hygroscopic growth. We define the
indirect effectas a reduction in the dust AOD due to the higher removal of the aged dust particles.
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.
Mira L. Pöhlker, Christopher Pöhlker, Florian Ditas, Thomas Klimach, Isabella Hrabe de Angelis, Alessandro Araújo, Joel Brito, Samara Carbone, Yafang Cheng, Xuguang Chi, Reiner Ditz, Sachin S. Gunthe, Jürgen Kesselmeier, Tobias Könemann, Jošt V. Lavrič, Scot T. Martin, Eugene Mikhailov, Daniel Moran-Zuloaga, Diana Rose, Jorge Saturno, Hang Su, Ryan Thalman, David Walter, Jian Wang, Stefan Wolff, Henrique M. J. Barbosa, Paulo Artaxo, Meinrat O. Andreae, and Ulrich Pöschl
Atmos. Chem. Phys., 16, 15709–15740, https://doi.org/10.5194/acp-16-15709-2016, https://doi.org/10.5194/acp-16-15709-2016, 2016
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The paper presents a systematic characterization of cloud condensation nuclei (CCN) concentration in the central Amazonian atmosphere. Our results show that the CCN population in this globally important ecosystem follows a pollution-related seasonal cycle, in which it mainly depends on changes in total aerosol size distribution and to a minor extent in the aerosol chemical composition. Our results allow an efficient modeling and prediction of the CCN population based on a novel approach.
Hannah Meusel, Uwe Kuhn, Andreas Reiffs, Chinmay Mallik, Hartwig Harder, Monica Martinez, Jan Schuladen, Birger Bohn, Uwe Parchatka, John N. Crowley, Horst Fischer, Laura Tomsche, Anna Novelli, Thorsten Hoffmann, Ruud H. H. Janssen, Oscar Hartogensis, Michael Pikridas, Mihalis Vrekoussis, Efstratios Bourtsoukidis, Bettina Weber, Jos Lelieveld, Jonathan Williams, Ulrich Pöschl, Yafang Cheng, and Hang Su
Atmos. Chem. Phys., 16, 14475–14493, https://doi.org/10.5194/acp-16-14475-2016, https://doi.org/10.5194/acp-16-14475-2016, 2016
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There are many studies which show discrepancies between modeled and measured nitrous acid (HONO, precursor of OH radical) in the troposphere but with no satisfactory explanation. Ideal conditions to study the unknown sources of HONO were found on Cyprus, a remote Mediterranean island. Budget analysis of trace gas measurements indicates a common source of NO and HONO, which is not related to anthropogenic activity and is most likely derived from biologic activity in soils and subsequent emission.
Dimitris Akritidis, Andrea Pozzer, Prodromos Zanis, Evangelos Tyrlis, Bojan Škerlak, Michael Sprenger, and Jos Lelieveld
Atmos. Chem. Phys., 16, 14025–14039, https://doi.org/10.5194/acp-16-14025-2016, https://doi.org/10.5194/acp-16-14025-2016, 2016
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We investigate the contribution of tropopause folds in the summertime tropospheric ozone pool over the eastern Mediterranean and the Middle East. For this purpose we use the EMAC atmospheric chemistry–climate model and a fold identification algorithm. A clear increase of ozone is found in the middle troposphere due to fold activity. The interannual variability of near-surface ozone over the eastern Mediterranean is related to that of both tropopause folds and ozone in the free troposphere.
Aristeidis K. Georgoulias, Georgia Alexandri, Konstantinos A. Kourtidis, Jos Lelieveld, Prodromos Zanis, Ulrich Pöschl, Robert Levy, Vassilis Amiridis, Eleni Marinou, and Athanasios Tsikerdekis
Atmos. Chem. Phys., 16, 13853–13884, https://doi.org/10.5194/acp-16-13853-2016, https://doi.org/10.5194/acp-16-13853-2016, 2016
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In this work, single pixel observations from MODIS Terra and Aqua are analyzed together with data from other satellite sensors, reanalysis projects and a chemistry–aerosol-transport model to study the spatiotemporal variability of different aerosol types. The results are in accordance with previous works and are a good reference for future studies in the area focusing on aerosols, clouds, radiation and the effects of particle pollution on human health.
Gavin J. Phillips, Jim Thieser, Mingjin Tang, Nicolas Sobanski, Gerhard Schuster, Johannes Fachinger, Frank Drewnick, Stephan Borrmann, Heinz Bingemer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 16, 13231–13249, https://doi.org/10.5194/acp-16-13231-2016, https://doi.org/10.5194/acp-16-13231-2016, 2016
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We use trace gas measurements (N2O5, ClNO2, NO3) and particle properties (surface area, nitrate content etc.) to derive uptake coefficients (the probability of removal from the gas-phase on a per-collision basis) for the interaction of N2O5 with ambient aerosol and also the efficiency of formation of ClNO2. The uptake coefficients show high variability but are reasonably well captured by parameterisations based on laboratory measurements.
Nicolas Sobanski, Jan Schuladen, Gerhard Schuster, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 9, 5103–5118, https://doi.org/10.5194/amt-9-5103-2016, https://doi.org/10.5194/amt-9-5103-2016, 2016
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We report the characteristics and performances of a cavity ring-down spectrometer (CRDS) designed for field measurements that uses light absorption at 662 and 405 nm to detect different reactive nitrogen species or group of species in the gas phase, either directly or after thermal decomposition. We report improvements compared to currently existing instruments, and describe the corrections applied to the raw data to account for chemical and optical interferences.
Jos Lelieveld, Sergey Gromov, Andrea Pozzer, and Domenico Taraborrelli
Atmos. Chem. Phys., 16, 12477–12493, https://doi.org/10.5194/acp-16-12477-2016, https://doi.org/10.5194/acp-16-12477-2016, 2016
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The self-cleaning capacity of the atmosphere is controlled by hydroxyl (OH) radicals in the troposphere. There are primary and secondary OH sources, the former through the photodissociation of ozone, the latter through OH recycling. We used a global model, showing that secondary sources are larger than assumed previously, which buffers OH. Complementary OH formation mechanisms in pristine and polluted environments, connected through transport of ozone, can maintain stable global OH levels.
A. M. Yáñez-Serrano, A. C. Nölscher, E. Bourtsoukidis, B. Derstroff, N. Zannoni, V. Gros, M. Lanza, J. Brito, S. M. Noe, E. House, C. N. Hewitt, B. Langford, E. Nemitz, T. Behrendt, J. Williams, P. Artaxo, M. O. Andreae, and J. Kesselmeier
Atmos. Chem. Phys., 16, 10965–10984, https://doi.org/10.5194/acp-16-10965-2016, https://doi.org/10.5194/acp-16-10965-2016, 2016
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This paper provides a general overview of methyl ethyl ketone (MEK) ambient observations in different ecosystems around the world in order to provide insights into the sources, sink and role of MEK in the atmosphere.
Jan Zörner, Marloes Penning de Vries, Steffen Beirle, Holger Sihler, Patrick R. Veres, Jonathan Williams, and Thomas Wagner
Atmos. Chem. Phys., 16, 9457–9487, https://doi.org/10.5194/acp-16-9457-2016, https://doi.org/10.5194/acp-16-9457-2016, 2016
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We present a top-down approach to infer and quantify rain-induced emission pulses of nitrogen oxides from soils using satellite-borne measurements of NO2. We found strong enhancements of NO2 induced by the first intense precipitation after prolonged droughts in many semi-arid regions of the world, in particular in the Sahel. Apart from the clear first-day peak, NO2 VCDs are moderately enhanced compared to background over the following 2 weeks suggesting potential further emissions.
Alexandra P. Tsimpidi, Vlassis A. Karydis, Spyros N. Pandis, and Jos Lelieveld
Atmos. Chem. Phys., 16, 8939–8962, https://doi.org/10.5194/acp-16-8939-2016, https://doi.org/10.5194/acp-16-8939-2016, 2016
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In this work we use a global chemistry climate model together with a comprehensive global AMS data set in order to provide valuable insights into the temporal and geographical variability of the contribution of the emitted particles and the chemically processed organic material from combustion sources to total OA. This study reveals the high importance of SOA from anthropogenic sources on global OA concentrations and identifies plausible sources of discrepancy between models and measurements.
Boris Bonn, Erika von Schneidemesser, Dorota Andrich, Jörn Quedenau, Holger Gerwig, Anja Lüdecke, Jürgen Kura, Axel Pietsch, Christian Ehlers, Dieter Klemp, Claudia Kofahl, Rainer Nothard, Andreas Kerschbaumer, Wolfgang Junkermann, Rüdiger Grote, Tobias Pohl, Konradin Weber, Birgit Lode, Philipp Schönberger, Galina Churkina, Tim M. Butler, and Mark G. Lawrence
Atmos. Chem. Phys., 16, 7785–7811, https://doi.org/10.5194/acp-16-7785-2016, https://doi.org/10.5194/acp-16-7785-2016, 2016
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The distribution of air pollutants (gases and particles) have been investigated in different environments in Potsdam, Germany. Remarkable variations of the pollutants have been observed for distances of tens of meters by bicycles, vans and aircraft. Vegetated areas caused reductions depending on the pollutants, the vegetation type and dimensions. Our measurements show the pollutants to be of predominantly local origin, resulting in a huge challenge for common models to resolve.
Swen Metzger, Benedikt Steil, Mohamed Abdelkader, Klaus Klingmüller, Li Xu, Joyce E. Penner, Christos Fountoukis, Athanasios Nenes, and Jos Lelieveld
Atmos. Chem. Phys., 16, 7213–7237, https://doi.org/10.5194/acp-16-7213-2016, https://doi.org/10.5194/acp-16-7213-2016, 2016
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We introduce an unique single parameter framework to efficiently parameterize the aerosol water uptake for mixtures of semi-volatile and non-volatile compounds, being entirely based on the single solute specific coefficient introduced in Metzger et al. (2012).
Klaus Klingmüller, Andrea Pozzer, Swen Metzger, Georgiy L. Stenchikov, and Jos Lelieveld
Atmos. Chem. Phys., 16, 5063–5073, https://doi.org/10.5194/acp-16-5063-2016, https://doi.org/10.5194/acp-16-5063-2016, 2016
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During the last decade, the Middle East experienced the strongest increase in atmospheric aerosol concentrations worldwide. Based on satellite observations, the present study corroborates this trend and reveals correlations with soil moisture and precipitation in and surrounding the Fertile Crescent. This suggests that the increasing drought conditions in this region have enhanced dust emissions, a tendency which is expected to be intensified by climate change.
N. Sobanski, M. J. Tang, J. Thieser, G. Schuster, D. Pöhler, H. Fischer, W. Song, C. Sauvage, J. Williams, J. Fachinger, F. Berkes, P. Hoor, U. Platt, J. Lelieveld, and J. N. Crowley
Atmos. Chem. Phys., 16, 4867–4883, https://doi.org/10.5194/acp-16-4867-2016, https://doi.org/10.5194/acp-16-4867-2016, 2016
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The nitrate radical (NO3) is an important nocturnal oxidant. By measuring NO3, its precursors (nitrogen dioxide and ozone) and several trace gases with which it reacts, we examined the chemical and meteorological factors influencing the lifetime of NO3 at a semi-rural mountain site. Unexpectedly long lifetimes, approaching 1 h, were observed on several nights and were associated with a low-lying residual layer. We discuss the role of other reactions that convert NO2 to NO3.
Jérôme Ogée, Joana Sauze, Jürgen Kesselmeier, Bernard Genty, Heidi Van Diest, Thomas Launois, and Lisa Wingate
Biogeosciences, 13, 2221–2240, https://doi.org/10.5194/bg-13-2221-2016, https://doi.org/10.5194/bg-13-2221-2016, 2016
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Estimates of photosynthesis and respiration at large scales are needed to improve our predictions of the global CO2 cycle. Carbonyl sulfide (OCS) has been proposed as a new tracer of photosynthesis, as it was shown that the uptake of OCS from leaves is nearly proportional to photosynthesis. But soils also exchange OCS with the atmosphere. Here we propose a mechanistic model of this exchange and show, using this new model, how we are able to explain several observed features of soil OCS fluxes.
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.
Shang Sun, Alexander Moravek, Lisa von der Heyden, Andreas Held, Matthias Sörgel, and Jürgen Kesselmeier
Atmos. Meas. Tech., 9, 599–617, https://doi.org/10.5194/amt-9-599-2016, https://doi.org/10.5194/amt-9-599-2016, 2016
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We present a dynamic twin-cuvette system for quantifying the trace gas exchange fluxes between plants and the atmosphere under controlled temperature, light, and humidity conditions. We found out that at a relative humidity of 40 %, the deposition velocity ratio of O3 and PAN was determined to be 0.45. At that humidity, the O3-deposition to the plant leaves was found to be only controlled by leaf stomata. For PAN, an additional resistance inhibited the uptake of PAN by the leaves.
J. Thieser, G. Schuster, J. Schuladen, G. J. Phillips, A. Reiffs, U. Parchatka, D. Pöhler, J. Lelieveld, and J. N. Crowley
Atmos. Meas. Tech., 9, 553–576, https://doi.org/10.5194/amt-9-553-2016, https://doi.org/10.5194/amt-9-553-2016, 2016
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We report on the use of thermal dissociation cavity ring-down spectroscopy to detect NO2, peroxy nitrates and alkyl nitrates. We present both laboratory studies that characterise the chemical formation and loss of NO2 in the heated inlets and also result from a first field deployment.
V. A. Karydis, A. P. Tsimpidi, A. Pozzer, M. Astitha, and J. Lelieveld
Atmos. Chem. Phys., 16, 1491–1509, https://doi.org/10.5194/acp-16-1491-2016, https://doi.org/10.5194/acp-16-1491-2016, 2016
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We provide an assessment of the chemical composition and global aerosol load of aerosol nitrate and determine the effect of mineral dust on its formation due to thermodynamical interactions. For this purpose we used an explicit geographical representation of the emitted soil particle size distribution and chemical composition. We conclude mineral dust aerosol chemistry is important for nitrate aerosol formation and significantly affects its global distribution, especially in the coarse mode.
M. O. Andreae, O. C. Acevedo, A. Araùjo, P. Artaxo, C. G. G. Barbosa, H. M. J. Barbosa, J. Brito, S. Carbone, X. Chi, B. B. L. Cintra, N. F. da Silva, N. L. Dias, C. Q. Dias-Júnior, F. Ditas, R. Ditz, A. F. L. Godoi, R. H. M. Godoi, M. Heimann, T. Hoffmann, J. Kesselmeier, T. Könemann, M. L. Krüger, J. V. Lavric, A. O. Manzi, A. P. Lopes, D. L. Martins, E. F. Mikhailov, D. Moran-Zuloaga, B. W. Nelson, A. C. Nölscher, D. Santos Nogueira, M. T. F. Piedade, C. Pöhlker, U. Pöschl, C. A. Quesada, L. V. Rizzo, C.-U. Ro, N. Ruckteschler, L. D. A. Sá, M. de Oliveira Sá, C. B. Sales, R. M. N. dos Santos, J. Saturno, J. Schöngart, M. Sörgel, C. M. de Souza, R. A. F. de Souza, H. Su, N. Targhetta, J. Tóta, I. Trebs, S. Trumbore, A. van Eijck, D. Walter, Z. Wang, B. Weber, J. Williams, J. Winderlich, F. Wittmann, S. Wolff, and A. M. Yáñez-Serrano
Atmos. Chem. Phys., 15, 10723–10776, https://doi.org/10.5194/acp-15-10723-2015, https://doi.org/10.5194/acp-15-10723-2015, 2015
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This paper describes the Amazon Tall Tower Observatory (ATTO), a new atmosphere-biosphere observatory located in the remote Amazon Basin. It presents results from ecosystem ecology, meteorology, trace gas, and aerosol measurements collected at the ATTO site during the first 3 years of operation.
M. Abdelkader, S. Metzger, R. E. Mamouri, M. Astitha, L. Barrie, Z. Levin, and J. Lelieveld
Atmos. Chem. Phys., 15, 9173–9189, https://doi.org/10.5194/acp-15-9173-2015, https://doi.org/10.5194/acp-15-9173-2015, 2015
H. G. Ouwersloot, A. Pozzer, B. Steil, H. Tost, and J. Lelieveld
Geosci. Model Dev., 8, 2435–2445, https://doi.org/10.5194/gmd-8-2435-2015, https://doi.org/10.5194/gmd-8-2435-2015, 2015
H. Fischer, A. Pozzer, T. Schmitt, P. Jöckel, T. Klippel, D. Taraborrelli, and J. Lelieveld
Atmos. Chem. Phys., 15, 6971–6980, https://doi.org/10.5194/acp-15-6971-2015, https://doi.org/10.5194/acp-15-6971-2015, 2015
K. Violaki, J. Sciare, J. Williams, A. R. Baker, M. Martino, and N. Mihalopoulos
Biogeosciences, 12, 3131–3140, https://doi.org/10.5194/bg-12-3131-2015, https://doi.org/10.5194/bg-12-3131-2015, 2015
S. Zheng, A. Pozzer, C. X. Cao, and J. Lelieveld
Atmos. Chem. Phys., 15, 5715–5725, https://doi.org/10.5194/acp-15-5715-2015, https://doi.org/10.5194/acp-15-5715-2015, 2015
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The present study uses aerosol optical depth as proxy to estimate 12 years of PM2.5 data for the Beijing central area and calculate the yearly premature mortality by different diseases attributable to PM2.5. The estimated average total mortality due to PM2.5 is about 5100 individuals/year for the period 2001--2012 in the Beijing central area, and the per capita mortality for all ages due to PM2.5 is around 15 per 10,000 person-years for the period 2010--2012.
D. Mogensen, R. Gierens, J. N. Crowley, P. Keronen, S. Smolander, A. Sogachev, A. C. Nölscher, L. Zhou, M. Kulmala, M. J. Tang, J. Williams, and M. Boy
Atmos. Chem. Phys., 15, 3909–3932, https://doi.org/10.5194/acp-15-3909-2015, https://doi.org/10.5194/acp-15-3909-2015, 2015
A. M. Yáñez-Serrano, A. C. Nölscher, J. Williams, S. Wolff, E. Alves, G. A. Martins, E. Bourtsoukidis, J. Brito, K. Jardine, P. Artaxo, and J. Kesselmeier
Atmos. Chem. Phys., 15, 3359–3378, https://doi.org/10.5194/acp-15-3359-2015, https://doi.org/10.5194/acp-15-3359-2015, 2015
E. Mesarchaki, C. Kräuter, K. E. Krall, M. Bopp, F. Helleis, J. Williams, and B. Jähne
Ocean Sci., 11, 121–138, https://doi.org/10.5194/os-11-121-2015, https://doi.org/10.5194/os-11-121-2015, 2015
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Our article presents successful gas exchange measurements obtained in a large-scale wind-wave tank. The adopted box model methodology, experimental produce and instrumentation are described in detail. For the first time, parallel measurements of total transfer velocities for 14 individual gases within a wide range of solubility have been achieved. Various wind speed conditions and the effect of surfactant layers have been investigated providing exciting results.
R. Oswald, M. Ermel, K. Hens, A. Novelli, H. G. Ouwersloot, P. Paasonen, T. Petäjä, M. Sipilä, P. Keronen, J. Bäck, R. Königstedt, Z. Hosaynali Beygi, H. Fischer, B. Bohn, D. Kubistin, H. Harder, M. Martinez, J. Williams, T. Hoffmann, I. Trebs, and M. Sörgel
Atmos. Chem. Phys., 15, 799–813, https://doi.org/10.5194/acp-15-799-2015, https://doi.org/10.5194/acp-15-799-2015, 2015
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Nitrous acid (HONO) is a key species in atmospheric photochemistry since the photolysis leads to the important hydroxyl radical (OH). Although the importance of HONO as a precursor of OH is known, the formation pathways of HONO, especially during daytime, are a major challenge in atmospheric science. We present a detailed analysis of sources and sinks for HONO in the atmosphere for a field measurement campaign in the boreal forest in Finland and wonder if there is really a source term missing.
C. E. Stockwell, P. R. Veres, J. Williams, and R. J. Yokelson
Atmos. Chem. Phys., 15, 845–865, https://doi.org/10.5194/acp-15-845-2015, https://doi.org/10.5194/acp-15-845-2015, 2015
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We used a high-resolution proton-transfer-reaction time-of-flight mass spectrometer to measure emissions from peat, crop residue, cooking fires, etc. We assigned > 80% of the mass of gas-phase organic compounds and much of it was secondary organic aerosol precursors. The open cooking emissions were much larger than from advanced cookstoves. Little-studied N-containing organic compounds accounted for 0.1-8.7% of the fuel N and may influence new particle formation.
A. P. Tsimpidi, V. A. Karydis, A. Pozzer, S. N. Pandis, and J. Lelieveld
Geosci. Model Dev., 7, 3153–3172, https://doi.org/10.5194/gmd-7-3153-2014, https://doi.org/10.5194/gmd-7-3153-2014, 2014
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A computationally efficient module for the description of OA composition and evolution in the atmosphere has been developed. This module subdivides OA into several compounds based on their source of origin and volatility, allowing the quantification of POA vs. SOA as well as biogenic vs. anthropogenic contributions to OA concentrations. Such fundamental information can shed light on long-term changes in OA abundance, and hence project the effects of OA on future air quality and climate.
K. Klingmüller, B. Steil, C. Brühl, H. Tost, and J. Lelieveld
Geosci. Model Dev., 7, 2503–2516, https://doi.org/10.5194/gmd-7-2503-2014, https://doi.org/10.5194/gmd-7-2503-2014, 2014
B. Bonn, E. Bourtsoukidis, T. S. Sun, H. Bingemer, L. Rondo, U. Javed, J. Li, R. Axinte, X. Li, T. Brauers, H. Sonderfeld, R. Koppmann, A. Sogachev, S. Jacobi, and D. V. Spracklen
Atmos. Chem. Phys., 14, 10823–10843, https://doi.org/10.5194/acp-14-10823-2014, https://doi.org/10.5194/acp-14-10823-2014, 2014
T. Behrendt, P. R. Veres, F. Ashuri, G. Song, M. Flanz, B. Mamtimin, M. Bruse, J. Williams, and F. X. Meixner
Biogeosciences, 11, 5463–5492, https://doi.org/10.5194/bg-11-5463-2014, https://doi.org/10.5194/bg-11-5463-2014, 2014
A. Novelli, K. Hens, C. Tatum Ernest, D. Kubistin, E. Regelin, T. Elste, C. Plass-Dülmer, M. Martinez, J. Lelieveld, and H. Harder
Atmos. Meas. Tech., 7, 3413–3430, https://doi.org/10.5194/amt-7-3413-2014, https://doi.org/10.5194/amt-7-3413-2014, 2014
H. Bozem, H. Fischer, C. Gurk, C. L. Schiller, U. Parchatka, R. Koenigstedt, A. Stickler, M. Martinez, H. Harder, D. Kubistin, J. Williams, G. Eerdekens, and J. Lelieveld
Atmos. Chem. Phys., 14, 8917–8931, https://doi.org/10.5194/acp-14-8917-2014, https://doi.org/10.5194/acp-14-8917-2014, 2014
D. Y. Chang, H. Tost, B. Steil, and J. Lelieveld
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-14-21975-2014, https://doi.org/10.5194/acpd-14-21975-2014, 2014
Preprint withdrawn
K. Hens, A. Novelli, M. Martinez, J. Auld, R. Axinte, B. Bohn, H. Fischer, P. Keronen, D. Kubistin, A. C. Nölscher, R. Oswald, P. Paasonen, T. Petäjä, E. Regelin, R. Sander, V. Sinha, M. Sipilä, D. Taraborrelli, C. Tatum Ernest, J. Williams, J. Lelieveld, and H. Harder
Atmos. Chem. Phys., 14, 8723–8747, https://doi.org/10.5194/acp-14-8723-2014, https://doi.org/10.5194/acp-14-8723-2014, 2014
P. R. Veres, T. Behrendt, A. Klapthor, F. X. Meixner, and J. Williams
Biogeosciences Discuss., https://doi.org/10.5194/bgd-11-12009-2014, https://doi.org/10.5194/bgd-11-12009-2014, 2014
Revised manuscript not accepted
A. K. Mishra, K. Klingmueller, E. Fredj, J. Lelieveld, Y. Rudich, and I. Koren
Atmos. Chem. Phys., 14, 7213–7231, https://doi.org/10.5194/acp-14-7213-2014, https://doi.org/10.5194/acp-14-7213-2014, 2014
E. Bourtsoukidis, J. Williams, J. Kesselmeier, S. Jacobi, and B. Bonn
Atmos. Chem. Phys., 14, 6495–6510, https://doi.org/10.5194/acp-14-6495-2014, https://doi.org/10.5194/acp-14-6495-2014, 2014
T. Christoudias, Y. Proestos, and J. Lelieveld
Atmos. Chem. Phys., 14, 4607–4616, https://doi.org/10.5194/acp-14-4607-2014, https://doi.org/10.5194/acp-14-4607-2014, 2014
G. W. Mann, K. S. Carslaw, C. L. Reddington, K. J. Pringle, M. Schulz, A. Asmi, D. V. Spracklen, D. A. Ridley, M. T. Woodhouse, L. A. Lee, K. Zhang, S. J. Ghan, R. C. Easter, X. Liu, P. Stier, Y. H. Lee, P. J. Adams, H. Tost, J. Lelieveld, S. E. Bauer, K. Tsigaridis, T. P. C. van Noije, A. Strunk, E. Vignati, N. Bellouin, M. Dalvi, C. E. Johnson, T. Bergman, H. Kokkola, K. von Salzen, F. Yu, G. Luo, A. Petzold, J. Heintzenberg, A. Clarke, J. A. Ogren, J. Gras, U. Baltensperger, U. Kaminski, S. G. Jennings, C. D. O'Dowd, R. M. Harrison, D. C. S. Beddows, M. Kulmala, Y. Viisanen, V. Ulevicius, N. Mihalopoulos, V. Zdimal, M. Fiebig, H.-C. Hansson, E. Swietlicki, and J. S. Henzing
Atmos. Chem. Phys., 14, 4679–4713, https://doi.org/10.5194/acp-14-4679-2014, https://doi.org/10.5194/acp-14-4679-2014, 2014
W. Song, M. Staudt, I. Bourgeois, and J. Williams
Biogeosciences, 11, 1435–1447, https://doi.org/10.5194/bg-11-1435-2014, https://doi.org/10.5194/bg-11-1435-2014, 2014
J. A. Adame, M. Martínez, M. Sorribas, P. J. Hidalgo, H. Harder, J.-M. Diesch, F. Drewnick, W. Song, J. Williams, V. Sinha, M. A. Hernández-Ceballos, J. Vilà-Guerau de Arellano, R. Sander, Z. Hosaynali-Beygi, H. Fischer, J. Lelieveld, and B. De la Morena
Atmos. Chem. Phys., 14, 2325–2342, https://doi.org/10.5194/acp-14-2325-2014, https://doi.org/10.5194/acp-14-2325-2014, 2014
C. Liu, S. Beirle, T. Butler, P. Hoor, C. Frankenberg, P. Jöckel, M. Penning de Vries, U. Platt, A. Pozzer, M. G. Lawrence, J. Lelieveld, H. Tost, and T. Wagner
Atmos. Chem. Phys., 14, 1717–1732, https://doi.org/10.5194/acp-14-1717-2014, https://doi.org/10.5194/acp-14-1717-2014, 2014
Y. F. Elshorbany, P. J. Crutzen, B. Steil, A. Pozzer, H. Tost, and J. Lelieveld
Atmos. Chem. Phys., 14, 1167–1184, https://doi.org/10.5194/acp-14-1167-2014, https://doi.org/10.5194/acp-14-1167-2014, 2014
D. Giannadaki, A. Pozzer, and J. Lelieveld
Atmos. Chem. Phys., 14, 957–968, https://doi.org/10.5194/acp-14-957-2014, https://doi.org/10.5194/acp-14-957-2014, 2014
P. Zanis, P. Hadjinicolaou, A. Pozzer, E. Tyrlis, S. Dafka, N. Mihalopoulos, and J. Lelieveld
Atmos. Chem. Phys., 14, 115–132, https://doi.org/10.5194/acp-14-115-2014, https://doi.org/10.5194/acp-14-115-2014, 2014
A. L. Corrigan, L. M. Russell, S. Takahama, M. Äijälä, M. Ehn, H. Junninen, J. Rinne, T. Petäjä, M. Kulmala, A. L. Vogel, T. Hoffmann, C. J. Ebben, F. M. Geiger, P. Chhabra, J. H. Seinfeld, D. R. Worsnop, W. Song, J. Auld, and J. Williams
Atmos. Chem. Phys., 13, 12233–12256, https://doi.org/10.5194/acp-13-12233-2013, https://doi.org/10.5194/acp-13-12233-2013, 2013
B. Bonn, S. Sun, W. Haunold, R. Sitals, E. van Beesel, L. dos Santos, B. Nillius, and S. Jacobi
Atmos. Meas. Tech., 6, 3407–3423, https://doi.org/10.5194/amt-6-3407-2013, https://doi.org/10.5194/amt-6-3407-2013, 2013
J. Yoon, A. Pozzer, P. Hoor, D. Y. Chang, S. Beirle, T. Wagner, S. Schloegl, J. Lelieveld, and H. M. Worden
Atmos. Chem. Phys., 13, 11307–11316, https://doi.org/10.5194/acp-13-11307-2013, https://doi.org/10.5194/acp-13-11307-2013, 2013
A. L. Vogel, M. Äijälä, A. L. Corrigan, H. Junninen, M. Ehn, T. Petäjä, D. R. Worsnop, M. Kulmala, L. M. Russell, J. Williams, and T. Hoffmann
Atmos. Chem. Phys., 13, 10933–10950, https://doi.org/10.5194/acp-13-10933-2013, https://doi.org/10.5194/acp-13-10933-2013, 2013
E. Regelin, H. Harder, M. Martinez, D. Kubistin, C. Tatum Ernest, H. Bozem, T. Klippel, Z. Hosaynali-Beygi, H. Fischer, R. Sander, P. Jöckel, R. Königstedt, and J. Lelieveld
Atmos. Chem. Phys., 13, 10703–10720, https://doi.org/10.5194/acp-13-10703-2013, https://doi.org/10.5194/acp-13-10703-2013, 2013
A. Bracho-Nunez, N. M. Knothe,, S. Welter, M. Staudt, W. R. Costa, M. A. R. Liberato, M. T. F. Piedade, and J. Kesselmeier
Biogeosciences, 10, 5855–5873, https://doi.org/10.5194/bg-10-5855-2013, https://doi.org/10.5194/bg-10-5855-2013, 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
M. D. Andrés-Hernández, D. Kartal, J. N. Crowley, V. Sinha, E. Regelin, M. Martínez-Harder, V. Nenakhov, J. Williams, H. Harder, H. Bozem, W. Song, J. Thieser, M. J. Tang, Z. Hosaynali Beigi, and J. P. Burrows
Atmos. Chem. Phys., 13, 5731–5749, https://doi.org/10.5194/acp-13-5731-2013, https://doi.org/10.5194/acp-13-5731-2013, 2013
C. Brühl, J. Lelieveld, M. Höpfner, and H. Tost
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-13-11395-2013, https://doi.org/10.5194/acpd-13-11395-2013, 2013
Revised manuscript not accepted
A. L. Vogel, M. Äijälä, M. Brüggemann, M. Ehn, H. Junninen, T. Petäjä, D. R. Worsnop, M. Kulmala, J. Williams, and T. Hoffmann
Atmos. Meas. Tech., 6, 431–443, https://doi.org/10.5194/amt-6-431-2013, https://doi.org/10.5194/amt-6-431-2013, 2013
G. J. Phillips, 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
C. Breuninger, F. X. Meixner, and J. Kesselmeier
Atmos. Chem. Phys., 13, 773–790, https://doi.org/10.5194/acp-13-773-2013, https://doi.org/10.5194/acp-13-773-2013, 2013
J. Lelieveld, M. G. Lawrence, and D. Kunkel
Atmos. Chem. Phys., 13, 31–34, https://doi.org/10.5194/acp-13-31-2013, https://doi.org/10.5194/acp-13-31-2013, 2013
A. Jugold, F. Althoff, M. Hurkuck, M. Greule, K. Lenhart, J. Lelieveld, and F. Keppler
Biogeosciences, 9, 5291–5301, https://doi.org/10.5194/bg-9-5291-2012, https://doi.org/10.5194/bg-9-5291-2012, 2012
A. C. Nölscher, V. Sinha, S. Bockisch, T. Klüpfel, and J. Williams
Atmos. Meas. Tech., 5, 2981–2992, https://doi.org/10.5194/amt-5-2981-2012, https://doi.org/10.5194/amt-5-2981-2012, 2012
Related subject area
Biogeochemistry: Air - Land Exchange
Evaluating adsorption isotherm models for determining the partitioning of ammonium between soil and soil pore water in environmental soil samples
Similar freezing spectra of particles in plant canopies and in the air at a high-altitude site
Anticorrelation of net uptake of atmospheric CO2 by the world ocean and terrestrial biosphere in current carbon cycle models
Impact of meteorological conditions on the biogenic volatile organic compound (BVOC) emission rate from eastern Mediterranean vegetation under drought
Monitoring cropland daily carbon dioxide exchange at field scales with Sentinel-2 satellite imagery
Compound soil and atmospheric drought (CSAD) events and CO2 fluxes of a mixed deciduous forest: the occurrence, impact, and temporal contribution of main drivers
The influence of plant water stress on vegetation–atmosphere exchanges: implications for ozone modelling
High interspecific variability in ice nucleation activity suggests pollen ice nucleators are incidental
Using automated machine learning for the upscaling of gross primary productivity
Aggregation of ice-nucleating macromolecules from Betula pendula pollen determines ice nucleation efficiency
Interpretability of negative latent heat fluxes from eddy covariance measurements in dry conditions
Forest-floor respiration, N2O fluxes, and CH4 fluxes in a subalpine spruce forest: drivers and annual budgets
Enhanced net CO2 exchange of a semideciduous forest in the southern Amazon due to diffuse radiation from biomass burning
Observational relationships between ammonia, carbon dioxide and water vapor under a wide range of meteorological and turbulent conditions: RITA-2021 campaign
Environmental controls of winter soil carbon dioxide fluxes in boreal and tundra environments
Origin of secondary fatty alcohols in atmospheric aerosols in a cool–temperate forest based on their mass size distributions
Sap flow and leaf gas exchange response to a drought and heatwave in urban green spaces in a Nordic city
Changes in biogenic volatile organic compound emissions in response to the El Niño–Southern Oscillation
Rethinking the deployment of static chambers for CO2 flux measurement in dry desert soils
Lichen species across Alaska produce highly active and stable ice nucleators
A differentiable, physics-informed ecosystem modeling and learning framework for large-scale inverse problems: demonstration with photosynthesis simulations
Snow–vegetation–atmosphere interactions in alpine tundra
Synergy between TROPOMI sun-induced chlorophyll fluorescence and MODIS spectral reflectance for understanding the dynamics of gross primary productivity at Integrated Carbon Observatory System (ICOS) ecosystem flux sites
Atmospheric deposition of reactive nitrogen to a deciduous forest in the southern Appalachian Mountains
Tropical cyclones facilitate recovery of forest leaf area from dry spells in East Asia
Minor contributions of daytime monoterpenes are major contributors to atmospheric reactivity
Using atmospheric observations to quantify annual biogenic carbon dioxide fluxes on the Alaska North Slope
Forest–atmosphere exchange of reactive nitrogen in a remote region – Part II: Modeling annual budgets
Growth and actual leaf temperature modulate CO2 responsiveness of monoterpene emissions from holm oak in opposite ways
Multi-year observations reveal a larger than expected autumn respiration signal across northeast Eurasia
Reviews and syntheses: VOC emissions from soil cover in boreal and temperate natural ecosystems of the Northern Hemisphere
Internal tree cycling and atmospheric archiving of mercury: examination with concentration and stable isotope analyses
Contrasting drought legacy effects on gross primary productivity in a mixed versus pure beech forest
CO2 and CH4 exchanges between moist moss tundra and atmosphere on Kapp Linné, Svalbard
Recent extreme drought events in the Amazon rainforest: assessment of different precipitation and evapotranspiration datasets and drought indicators
Variability and uncertainty in flux-site-scale net ecosystem exchange simulations based on machine learning and remote sensing: a systematic evaluation
Update of a biogeochemical model with process-based algorithms to predict ammonia volatilization from fertilized cultivated uplands and rice paddy fields
Massive warming-induced carbon loss from subalpine grassland soils in an altitudinal transplantation experiment
Climatic variation drives loss and restructuring of carbon and nitrogen in boreal forest wildfire
Gaps in network infrastructure limit our understanding of biogenic methane emissions for the United States
Changes of the aerodynamic characteristics of a flux site after an extensive windthrow
Carbon sequestration potential of street tree plantings in Helsinki
Technical note: Incorporating expert domain knowledge into causal structure discovery workflows
Sensitivity of biomass burning emissions estimates to land surface information
A convolutional neural network for spatial downscaling of satellite-based solar-induced chlorophyll fluorescence (SIFnet)
Influence of plant ecophysiology on ozone dry deposition: comparing between multiplicative and photosynthesis-based dry deposition schemes and their responses to rising CO2 level
Modeling the interinfluence of fertilizer-induced NH3 emission, nitrogen deposition, and aerosol radiative effects using modified CESM2
Physiological and climate controls on foliar mercury uptake by European tree species
Radiation, soil water content, and temperature effects on carbon cycling in an alpine swamp meadow of the northeastern Qinghai–Tibetan Plateau
Representativeness assessment of the pan-Arctic eddy covariance site network and optimized future enhancements
Matthew G. Davis, Kevin Yan, and Jennifer G. Murphy
Biogeosciences, 21, 5381–5392, https://doi.org/10.5194/bg-21-5381-2024, https://doi.org/10.5194/bg-21-5381-2024, 2024
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Ammonia applied as fertilizer can volatilize into the atmosphere. This can threaten vulnerable ecosystems and human health. We investigated the partitioning of ammonia between an immobile adsorbed phase and mobile aqueous phase using several adsorption models. Using the Temkin model we determined that previous approaches to this issue may overestimate the quantity available for exchange by a factor of 5–20, suggesting that ammonia emissions from soil may be overestimated.
Annika Einbock and Franz Conen
Biogeosciences, 21, 5219–5231, https://doi.org/10.5194/bg-21-5219-2024, https://doi.org/10.5194/bg-21-5219-2024, 2024
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A small fraction of particles found at great heights in the atmosphere can freeze cloud droplets at temperatures of ≥ −10 °C and thus influence cloud properties. We provide a novel type of evidence that plant canopies are a major source of such biological ice-nucleating particles in the air above the Alps, potentially affecting mixed-phase cloud development.
Stephen E. Schwartz
Biogeosciences, 21, 5045–5057, https://doi.org/10.5194/bg-21-5045-2024, https://doi.org/10.5194/bg-21-5045-2024, 2024
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Anticorrelation in uptake of atmospheric CO2 following pulse emission or abrupt cessation of emissions is examined in two key model intercomparison studies. In both studies net transfer coefficients from the atmosphere to the world ocean and the terrestrial biosphere are anticorrelated across models, reducing inter-model diversity in decrease of atmospheric CO2 following the perturbation, increasing uncertainties of global warming potentials and consequences of prospective emission reductions.
Qian Li, Gil Lerner, Einat Bar, Efraim Lewinsohn, and Eran Tas
Biogeosciences, 21, 4133–4147, https://doi.org/10.5194/bg-21-4133-2024, https://doi.org/10.5194/bg-21-4133-2024, 2024
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Our research indicates that instantaneous changes in meteorological parameters better reflect drought-induced changes in the emission rates of biogenic volatile organic compounds (BVOCs) from natural vegetation than their absolute values. However, following a small amount of irrigation, this trend became more moderate or reversed, accompanied by a dramatic increase in BVOC emission rates. These findings advance our understanding of BVOC emissions under climate change.
Pia Gottschalk, Aram Kalhori, Zhan Li, Christian Wille, and Torsten Sachs
Biogeosciences, 21, 3593–3616, https://doi.org/10.5194/bg-21-3593-2024, https://doi.org/10.5194/bg-21-3593-2024, 2024
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To improve the accuracy of spatial carbon exchange estimates, we evaluated simple linear models for net ecosystem exchange (NEE) and gross primary productivity (GPP) and how they can be used to upscale the CO2 exchange of agricultural fields. The models are solely driven by Sentinel-2-derived vegetation indices (VIs). Evaluations show that different VIs have variable power to estimate NEE and GPP of crops in different years. The overall performance is as good as results from complex crop models.
Liliana Scapucci, Ankit Shekhar, Sergio Aranda-Barranco, Anastasiia Bolshakova, Lukas Hörtnagl, Mana Gharun, and Nina Buchmann
Biogeosciences, 21, 3571–3592, https://doi.org/10.5194/bg-21-3571-2024, https://doi.org/10.5194/bg-21-3571-2024, 2024
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Forests face increased exposure to “compound soil and atmospheric drought” (CSAD) events due to global warming. We examined the impacts and drivers of CO2 fluxes during CSAD events at multiple layers of a deciduous forest over 18 years. Results showed reduced net ecosystem productivity and forest-floor respiration during CSAD events, mainly driven by soil and atmospheric drought. This unpredictability in forest CO2 fluxes jeopardises reforestation projects aimed at mitigating CO2 emissions.
Tamara Emmerichs, Yen-Sen Lu, and Domenico Taraborrelli
Biogeosciences, 21, 3251–3269, https://doi.org/10.5194/bg-21-3251-2024, https://doi.org/10.5194/bg-21-3251-2024, 2024
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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 into the atmosphere and thus significantly impacts the representation of weather as well as air quality. The newly implemented response function reduces this process and has a better comparison with satellite observations. This yields a higher intensity of unusual warm periods and higher production of air pollutants.
Nina L. H. Kinney, Charles A. Hepburn, Matthew I. Gibson, Daniel Ballesteros, and Thomas F. Whale
Biogeosciences, 21, 3201–3214, https://doi.org/10.5194/bg-21-3201-2024, https://doi.org/10.5194/bg-21-3201-2024, 2024
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Molecules released from plant pollen induce the formation of ice from supercooled water at temperatures warm enough to suggest an underlying function for this activity. In this study we show that ice nucleators are ubiquitous in pollen. We suggest the molecules responsible fulfil some unrelated biological function and nucleate ice incidentally. The ubiquity of ice-nucleating molecules in pollen and particularly active examples reveal a greater potential for pollen to impact weather and climate.
Max Gaber, Yanghui Kang, Guy Schurgers, and Trevor Keenan
Biogeosciences, 21, 2447–2472, https://doi.org/10.5194/bg-21-2447-2024, https://doi.org/10.5194/bg-21-2447-2024, 2024
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Gross primary productivity (GPP) describes the photosynthetic carbon assimilation, which plays a vital role in the carbon cycle. We can measure GPP locally, but producing larger and continuous estimates is challenging. Here, we present an approach to extrapolate GPP to a global scale using satellite imagery and automated machine learning. We benchmark different models and predictor variables and achieve an estimate that can capture 75 % of the variation in GPP.
Florian Wieland, Nadine Bothen, Ralph Schwidetzky, Teresa M. Seifried, Paul Bieber, Ulrich Pöschl, Konrad Meister, Mischa Bonn, Janine Fröhlich-Nowoisky, and Hinrich Grothe
EGUsphere, https://doi.org/10.5194/egusphere-2024-752, https://doi.org/10.5194/egusphere-2024-752, 2024
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Betula pendula is a widespread birch tree species containing ice nucleation agents that can trigger the freezing of cloud droplets, and thereby alter the evolution of clouds. Our study identifies three distinct ice-nucleating macromolecules (INMs) and aggregates of varying size that can nucleate ice at temperatures of up to -5.4 °C. Our findings suggest that these vegetation-derived particles may influence atmospheric processes, weather, and climate stronger than previously thought.
Sinikka J. Paulus, Rene Orth, Sung-Ching Lee, Anke Hildebrandt, Martin Jung, Jacob A. Nelson, Tarek Sebastian El-Madany, Arnaud Carrara, Gerardo Moreno, Matthias Mauder, Jannis Groh, Alexander Graf, Markus Reichstein, and Mirco Migliavacca
Biogeosciences, 21, 2051–2085, https://doi.org/10.5194/bg-21-2051-2024, https://doi.org/10.5194/bg-21-2051-2024, 2024
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Porous materials are known to reversibly trap water from the air, even at low humidity. However, this behavior is poorly understood for soils. In this analysis, we test whether eddy covariance is able to measure the so-called adsorption of atmospheric water vapor by soils. We find that this flux occurs frequently during dry nights in a Mediterranean ecosystem, while EC detects downwardly directed vapor fluxes. These results can help to map moisture uptake globally.
Luana Krebs, Susanne Burri, Iris Feigenwinter, Mana Gharun, Philip Meier, and Nina Buchmann
Biogeosciences, 21, 2005–2028, https://doi.org/10.5194/bg-21-2005-2024, https://doi.org/10.5194/bg-21-2005-2024, 2024
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This study explores year-round forest-floor greenhouse gas (GHG) fluxes in a Swiss spruce forest. Soil temperature and snow depth affected forest-floor respiration, while CH4 uptake was linked to snow cover. Negligible N2O fluxes were observed. In 2022, a warm year, CO2 emissions notably increased. The study suggests rising forest-floor GHG emissions due to climate change, impacting carbon sink behavior. Thus, for future forest management, continuous year-round GHG flux measurements are crucial.
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.
Ruben B. Schulte, Jordi Vilà-Guerau de Arellano, Susanna Rutledge-Jonker, Shelley van der Graaf, Jun Zhang, and Margreet C. van Zanten
Biogeosciences, 21, 557–574, https://doi.org/10.5194/bg-21-557-2024, https://doi.org/10.5194/bg-21-557-2024, 2024
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We analyzed measurements with the aim of finding relations between the surface atmosphere exchange of NH3 and the CO2 uptake and transpiration by vegetation. We found a high correlation of daytime NH3 emissions with both latent heat flux and photosynthetically active radiation. Very few simultaneous measurements of NH3, CO2 fluxes and meteorological variables exist at sub-diurnal timescales. This study paves the way to finding more robust relations between the NH3 exchange flux and CO2 uptake.
Alex Mavrovic, Oliver Sonnentag, Juha Lemmetyinen, Carolina Voigt, Nick Rutter, Paul Mann, Jean-Daniel Sylvain, and Alexandre Roy
Biogeosciences, 20, 5087–5108, https://doi.org/10.5194/bg-20-5087-2023, https://doi.org/10.5194/bg-20-5087-2023, 2023
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We present an analysis of soil CO2 emissions in boreal and tundra regions during the non-growing season. We show that when the soil is completely frozen, soil temperature is the main control on CO2 emissions. When the soil is around the freezing point, with a mix of liquid water and ice, the liquid water content is the main control on CO2 emissions. This study highlights that the vegetation–snow–soil interactions must be considered to understand soil CO2 emissions during the non-growing season.
Yuhao Cui, Eri Tachibana, Kimitaka Kawamura, and Yuzo Miyazaki
Biogeosciences, 20, 4969–4980, https://doi.org/10.5194/bg-20-4969-2023, https://doi.org/10.5194/bg-20-4969-2023, 2023
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Fatty alcohols (FAs) are major components of surface lipids in plant leaves and serve as surface-active aerosols. Our study on the aerosol size distributions in a forest suggests that secondary FAs (SFAs) originated from plant waxes and that leaf senescence status is likely an important factor controlling the size distribution of SFAs. This study provides new insights into the sources of primary biological aerosol particles (PBAPs) and their effects on the aerosol ice nucleation activity.
Joyson Ahongshangbam, Liisa Kulmala, Jesse Soininen, Yasmin Frühauf, Esko Karvinen, Yann Salmon, Anna Lintunen, Anni Karvonen, and Leena Järvi
Biogeosciences, 20, 4455–4475, https://doi.org/10.5194/bg-20-4455-2023, https://doi.org/10.5194/bg-20-4455-2023, 2023
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Urban vegetation is important for removing urban CO2 emissions and cooling. We studied the response of urban trees' functions (photosynthesis and transpiration) to a heatwave and drought at four urban green areas in the city of Helsinki. We found that tree water use was increased during heatwave and drought periods, but there was no change in the photosynthesis rates. The heat and drought conditions were severe at the local scale but were not excessive enough to restrict urban trees' functions.
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.
Nadav Bekin and Nurit Agam
Biogeosciences, 20, 3791–3802, https://doi.org/10.5194/bg-20-3791-2023, https://doi.org/10.5194/bg-20-3791-2023, 2023
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The mechanisms of soil CO2 flux in dry desert soils are not fully understood. Yet studies conducted in desert ecosystems rarely discuss potential errors related to using the commonly used flux chambers in dry and bare soils. In our study, the conventional deployment practice of the chambers underestimated the instantaneous CO2 flux by up to 50 % and the total daily CO2 uptake by 35 %. This suggests that desert soils are a larger carbon sink than previously reported.
Rosemary J. Eufemio, Ingrid de Almeida Ribeiro, Todd L. Sformo, Gary A. Laursen, Valeria Molinero, Janine Fröhlich-Nowoisky, Mischa Bonn, and Konrad Meister
Biogeosciences, 20, 2805–2812, https://doi.org/10.5194/bg-20-2805-2023, https://doi.org/10.5194/bg-20-2805-2023, 2023
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Lichens, the dominant vegetation in the Arctic, contain ice nucleators (INs) that enable freezing close to 0°C. Yet the abundance, diversity, and function of lichen INs is unknown. Our screening of lichens across Alaska reveal that most species have potent INs. We find that lichens contain two IN populations which retain activity under environmentally relevant conditions. The ubiquity and stability of lichen INs suggest that they may have considerable impacts on local atmospheric patterns.
Doaa Aboelyazeed, Chonggang Xu, Forrest M. Hoffman, Jiangtao Liu, Alex W. Jones, Chris Rackauckas, Kathryn Lawson, and Chaopeng Shen
Biogeosciences, 20, 2671–2692, https://doi.org/10.5194/bg-20-2671-2023, https://doi.org/10.5194/bg-20-2671-2023, 2023
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Photosynthesis is critical for life and has been affected by the changing climate. Many parameters come into play while modeling, but traditional calibration approaches face many issues. Our framework trains coupled neural networks to provide parameters to a photosynthesis model. Using big data, we independently found parameter values that were correlated with those in the literature while giving higher correlation and reduced biases in photosynthesis rates.
Norbert Pirk, Kristoffer Aalstad, Yeliz A. Yilmaz, Astrid Vatne, Andrea L. Popp, Peter Horvath, Anders Bryn, Ane Victoria Vollsnes, Sebastian Westermann, Terje Koren Berntsen, Frode Stordal, and Lena Merete Tallaksen
Biogeosciences, 20, 2031–2047, https://doi.org/10.5194/bg-20-2031-2023, https://doi.org/10.5194/bg-20-2031-2023, 2023
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We measured the land–atmosphere exchange of CO2 and water vapor in alpine Norway over 3 years. The extremely snow-rich conditions in 2020 reduced the total annual evapotranspiration to 50 % and reduced the growing-season carbon assimilation to turn the ecosystem from a moderate annual carbon sink to an even stronger source. Our analysis suggests that snow cover anomalies are driving the most consequential short-term responses in this ecosystem’s functioning.
Hamadou Balde, Gabriel Hmimina, Yves Goulas, Gwendal Latouche, and Kamel Soudani
Biogeosciences, 20, 1473–1490, https://doi.org/10.5194/bg-20-1473-2023, https://doi.org/10.5194/bg-20-1473-2023, 2023
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This study focuses on the relationship between sun-induced chlorophyll fluorescence (SIF) and ecosystem gross primary productivity (GPP) across the ICOS European flux tower network. It shows that SIF, coupled with reflectance observations, explains over 80 % of the GPP variability across diverse ecosystems but fails to bring new information compared to reflectance alone at coarse spatial scales (~5 km). These findings have applications in agriculture and ecophysiological studies.
John T. Walker, Xi Chen, Zhiyong Wu, Donna Schwede, Ryan Daly, Aleksandra Djurkovic, A. Christopher Oishi, Eric Edgerton, Jesse Bash, Jennifer Knoepp, Melissa Puchalski, John Iiames, and Chelcy F. Miniat
Biogeosciences, 20, 971–995, https://doi.org/10.5194/bg-20-971-2023, https://doi.org/10.5194/bg-20-971-2023, 2023
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Better estimates of atmospheric nitrogen (N) deposition are needed to accurately assess ecosystem risk and impacts from deposition of nutrients and acidity. Using measurements and modeling, we estimate total N deposition of 6.7 kg N ha−1 yr−1 at a forest site in the southern Appalachian Mountains, a region sensitive to atmospheric deposition. Reductions in deposition of reduced forms of N (ammonia and ammonium) will be needed to meet the lowest estimates of N critical loads for the region.
Yi-Ying Chen and Sebastiaan Luyssaert
Biogeosciences, 20, 349–363, https://doi.org/10.5194/bg-20-349-2023, https://doi.org/10.5194/bg-20-349-2023, 2023
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Tropical cyclones are typically assumed to be associated with ecosystem damage. This study challenges this assumption and suggests that instead of reducing leaf area, cyclones in East Asia may increase leaf area by alleviating water stress.
Deborah F. McGlynn, Graham Frazier, Laura E. R. Barry, Manuel T. Lerdau, Sally E. Pusede, and Gabriel Isaacman-VanWertz
Biogeosciences, 20, 45–55, https://doi.org/10.5194/bg-20-45-2023, https://doi.org/10.5194/bg-20-45-2023, 2023
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Using a custom-made gas chromatography flame ionization detector, 2 years of speciated hourly biogenic volatile organic compound data were collected in a forest in central Virginia. We identify diurnal and seasonal variability in the data, which is shown to impact atmospheric oxidant budgets. A comparison with emission models identified discrepancies with implications for model outcomes. We suggest increased monitoring of speciated biogenic volatile organic compounds to improve modeled results.
Luke D. Schiferl, Jennifer D. Watts, Erik J. L. Larson, Kyle A. Arndt, Sébastien C. Biraud, Eugénie S. Euskirchen, Jordan P. Goodrich, John M. Henderson, Aram Kalhori, Kathryn McKain, Marikate E. Mountain, J. William Munger, Walter C. Oechel, Colm Sweeney, Yonghong Yi, Donatella Zona, and Róisín Commane
Biogeosciences, 19, 5953–5972, https://doi.org/10.5194/bg-19-5953-2022, https://doi.org/10.5194/bg-19-5953-2022, 2022
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As the Arctic rapidly warms, vast stores of thawing permafrost could release carbon dioxide (CO2) into the atmosphere. We combined observations of atmospheric CO2 concentrations from aircraft and a tower with observed CO2 fluxes from tundra ecosystems and found that the Alaskan North Slope in not a consistent source nor sink of CO2. Our study shows the importance of using both site-level and atmospheric measurements to constrain regional net CO2 fluxes and improve biogenic processes in models.
Pascal Wintjen, Frederik Schrader, Martijn Schaap, Burkhard Beudert, Richard Kranenburg, and Christian Brümmer
Biogeosciences, 19, 5287–5311, https://doi.org/10.5194/bg-19-5287-2022, https://doi.org/10.5194/bg-19-5287-2022, 2022
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For the first time, we compared four methods for estimating the annual dry deposition of total reactive nitrogen into a low-polluted forest ecosystem. In our analysis, we used 2.5 years of flux measurements, an in situ modeling approach, a large-scale chemical transport model (CTM), and canopy budget models. Annual nitrogen dry deposition budgets ranged between 4.3 and 6.7 kg N ha−1 a−1, depending on the applied method.
Michael Staudt, Juliane Daussy, Joseph Ingabire, and Nafissa Dehimeche
Biogeosciences, 19, 4945–4963, https://doi.org/10.5194/bg-19-4945-2022, https://doi.org/10.5194/bg-19-4945-2022, 2022
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We studied the short- and long-term effects of CO2 as a function of temperature on monoterpene emissions from holm oak. Similarly to isoprene, emissions decreased non-linearly with increasing CO2, with no differences among compounds and chemotypes. The CO2 response was modulated by actual leaf and growth temperature but not by growth CO2. Estimates of annual monoterpene release under double CO2 suggest that CO2 inhibition does not offset the increase in emissions due to expected warming.
Brendan Byrne, Junjie Liu, Yonghong Yi, Abhishek Chatterjee, Sourish Basu, Rui Cheng, Russell Doughty, Frédéric Chevallier, Kevin W. Bowman, Nicholas C. Parazoo, David Crisp, Xing Li, Jingfeng Xiao, Stephen Sitch, Bertrand Guenet, Feng Deng, Matthew S. Johnson, Sajeev Philip, Patrick C. McGuire, and Charles E. Miller
Biogeosciences, 19, 4779–4799, https://doi.org/10.5194/bg-19-4779-2022, https://doi.org/10.5194/bg-19-4779-2022, 2022
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Plants draw CO2 from the atmosphere during the growing season, while respiration releases CO2 to the atmosphere throughout the year, driving seasonal variations in atmospheric CO2 that can be observed by satellites, such as the Orbiting Carbon Observatory 2 (OCO-2). Using OCO-2 XCO2 data and space-based constraints on plant growth, we show that permafrost-rich northeast Eurasia has a strong seasonal release of CO2 during the autumn, hinting at an unexpectedly large respiration signal from soils.
Valery A. Isidorov and Andrej A. Zaitsev
Biogeosciences, 19, 4715–4746, https://doi.org/10.5194/bg-19-4715-2022, https://doi.org/10.5194/bg-19-4715-2022, 2022
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Biogenic volatile organic compounds (VOCs) play a critical role in earth-system processes: they are
main playersin the formation of tropospheric O3 and secondary aerosols, which have a significant impact on climate, human health and crops. A complex mixture of VOCs, formed as a result of physicochemical and biological processes, is released into the atmosphere from the forest floor. This review presents data on the composition of VOCs and contribution of various processes to their emissions.
David S. McLagan, Harald Biester, Tomas Navrátil, Stephan M. Kraemer, and Lorenz Schwab
Biogeosciences, 19, 4415–4429, https://doi.org/10.5194/bg-19-4415-2022, https://doi.org/10.5194/bg-19-4415-2022, 2022
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Spruce and larch trees are effective archiving species for historical atmospheric mercury using growth rings of bole wood. Mercury stable isotope analysis proved an effective tool to characterise industrial mercury signals and assess mercury uptake pathways (leaf uptake for both wood and bark) and mercury cycling within the trees. These data detail important information for understanding the mercury biogeochemical cycle particularly in forest systems.
Xin Yu, René Orth, Markus Reichstein, Michael Bahn, Anne Klosterhalfen, Alexander Knohl, Franziska Koebsch, Mirco Migliavacca, Martina Mund, Jacob A. Nelson, Benjamin D. Stocker, Sophia Walther, and Ana Bastos
Biogeosciences, 19, 4315–4329, https://doi.org/10.5194/bg-19-4315-2022, https://doi.org/10.5194/bg-19-4315-2022, 2022
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Identifying drought legacy effects is challenging because they are superimposed on variability driven by climate conditions in the recovery period. We develop a residual-based approach to quantify legacies on gross primary productivity (GPP) from eddy covariance data. The GPP reduction due to legacy effects is comparable to the concurrent effects at two sites in Germany, which reveals the importance of legacy effects. Our novel methodology can be used to quantify drought legacies elsewhere.
Anders Lindroth, Norbert Pirk, Ingibjörg S. Jónsdóttir, Christian Stiegler, Leif Klemedtsson, and Mats B. Nilsson
Biogeosciences, 19, 3921–3934, https://doi.org/10.5194/bg-19-3921-2022, https://doi.org/10.5194/bg-19-3921-2022, 2022
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We measured the fluxes of carbon dioxide and methane between a moist moss tundra and the atmosphere on Svalbard in order to better understand how such ecosystems are affecting the climate and vice versa. We found that the system was a small sink of carbon dioxide and a small source of methane. These fluxes are small in comparison with other tundra ecosystems in the high Arctic. Analysis of temperature sensitivity showed that respiration was more sensitive than photosynthesis above about 6 ℃.
Phillip Papastefanou, Christian S. Zang, Zlatan Angelov, Aline Anderson de Castro, Juan Carlos Jimenez, Luiz Felipe Campos De Rezende, Romina C. Ruscica, Boris Sakschewski, Anna A. Sörensson, Kirsten Thonicke, Carolina Vera, Nicolas Viovy, Celso Von Randow, and Anja Rammig
Biogeosciences, 19, 3843–3861, https://doi.org/10.5194/bg-19-3843-2022, https://doi.org/10.5194/bg-19-3843-2022, 2022
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The Amazon rainforest has been hit by multiple severe drought events. In this study, we assess the severity and spatial extent of the extreme drought years 2005, 2010 and 2015/16 in the Amazon. Using nine different precipitation datasets and three drought indicators we find large differences in drought stress across the Amazon region. We conclude that future studies should use multiple rainfall datasets and drought indicators when estimating the impact of drought stress in the Amazon region.
Haiyang Shi, Geping Luo, Olaf Hellwich, Mingjuan Xie, Chen Zhang, Yu Zhang, Yuangang Wang, Xiuliang Yuan, Xiaofei Ma, Wenqiang Zhang, Alishir Kurban, Philippe De Maeyer, and Tim Van de Voorde
Biogeosciences, 19, 3739–3756, https://doi.org/10.5194/bg-19-3739-2022, https://doi.org/10.5194/bg-19-3739-2022, 2022
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A number of studies have been conducted by using machine learning approaches to simulate carbon fluxes. We performed a meta-analysis of these net ecosystem exchange (NEE) simulations. Random forests and support vector machines performed better than other algorithms. Models with larger timescales had a lower accuracy. For different plant functional types (PFTs), there were significant differences in the predictors used and their effects on model accuracy.
Siqi Li, Wei Zhang, Xunhua Zheng, Yong Li, Shenghui Han, Rui Wang, Kai Wang, Zhisheng Yao, Chunyan Liu, and Chong Zhang
Biogeosciences, 19, 3001–3019, https://doi.org/10.5194/bg-19-3001-2022, https://doi.org/10.5194/bg-19-3001-2022, 2022
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The CNMM–DNDC model was modified to simulate ammonia volatilization (AV) from croplands. AV from cultivated uplands followed the first-order kinetics, which was jointly regulated by the factors of soil properties and meteorological conditions. AV simulation from rice paddy fields was improved by incorporating Jayaweera–Mikkelsen mechanisms. The modified model performed well in simulating the observed cumulative AV measured from 63 fertilization events in China.
Matthias Volk, Matthias Suter, Anne-Lena Wahl, and Seraina Bassin
Biogeosciences, 19, 2921–2937, https://doi.org/10.5194/bg-19-2921-2022, https://doi.org/10.5194/bg-19-2921-2022, 2022
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Because soils are an important sink for greenhouse gasses, we subjected sub-alpine grassland to a six-level climate change treatment.
Two independent methods showed that at warming > 1.5 °C the grassland ecosystem lost ca. 14 % or ca. 1 kg C m−2 in 5 years.
This shrinking of the terrestrial C sink implies a substantial positive feedback to the atmospheric greenhouse effect.
It is likely that this dramatic C loss is a transient effect before a new, climate-adjusted steady state is reached.
Johan A. Eckdahl, Jeppe A. Kristensen, and Daniel B. Metcalfe
Biogeosciences, 19, 2487–2506, https://doi.org/10.5194/bg-19-2487-2022, https://doi.org/10.5194/bg-19-2487-2022, 2022
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This study found climate to be a driving force for increasing per area emissions of greenhouse gases and removal of important nutrients from high-latitude forests due to wildfire. It used detailed direct measurements over a large area to uncover patterns and mechanisms of restructuring of forest carbon and nitrogen pools that are extrapolatable to larger regions. It also takes a step forward in filling gaps in global knowledge of northern forest response to climate-change-strengthened wildfires.
Sparkle L. Malone, Youmi Oh, Kyle A. Arndt, George Burba, Roisin Commane, Alexandra R. Contosta, Jordan P. Goodrich, Henry W. Loescher, Gregory Starr, and Ruth K. Varner
Biogeosciences, 19, 2507–2522, https://doi.org/10.5194/bg-19-2507-2022, https://doi.org/10.5194/bg-19-2507-2022, 2022
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To understand the CH4 flux potential of natural ecosystems and agricultural lands in the United States of America, a multi-scale CH4 observation network focused on CH4 flux rates, processes, and scaling methods is required. This can be achieved with a network of ground-based observations that are distributed based on climatic regions and land cover.
Bruna R. F. Oliveira, Jan J. Keizer, and Thomas Foken
Biogeosciences, 19, 2235–2243, https://doi.org/10.5194/bg-19-2235-2022, https://doi.org/10.5194/bg-19-2235-2022, 2022
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This study analyzes the impacts of this windthrow on the aerodynamic characteristics of zero-plane displacement and roughness length and, ultimately, their implications for the turbulent fluxes. The turbulent fluxes were only affected to a minor degree by the windthrow, but the footprint area of the flux tower changed markedly so that the target area of the measurements had to be redetermined.
Minttu Havu, Liisa Kulmala, Pasi Kolari, Timo Vesala, Anu Riikonen, and Leena Järvi
Biogeosciences, 19, 2121–2143, https://doi.org/10.5194/bg-19-2121-2022, https://doi.org/10.5194/bg-19-2121-2022, 2022
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The carbon sequestration potential of two street tree species and the soil beneath them was quantified with the urban land surface model SUEWS and the soil carbon model Yasso. The street tree plantings turned into a modest sink of carbon from the atmosphere after 14 years. Overall, the results indicate the importance of soil in urban carbon sequestration estimations, as soil respiration exceeded the carbon uptake in the early phase, due to the high initial carbon loss from the soil.
Jarmo Mäkelä, Laila Melkas, Ivan Mammarella, Tuomo Nieminen, Suyog Chandramouli, Rafael Savvides, and Kai Puolamäki
Biogeosciences, 19, 2095–2099, https://doi.org/10.5194/bg-19-2095-2022, https://doi.org/10.5194/bg-19-2095-2022, 2022
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Causal structure discovery algorithms have been making headway into Earth system sciences, and they can be used to increase our understanding on biosphere–atmosphere interactions. In this paper we present a procedure on how to utilize prior knowledge of the domain experts together with these algorithms in order to find more robust causal structure models. We also demonstrate how to avoid pitfalls such as over-fitting and concept drift during this process.
Makoto Saito, Tomohiro Shiraishi, Ryuichi Hirata, Yosuke Niwa, Kazuyuki Saito, Martin Steinbacher, Doug Worthy, and Tsuneo Matsunaga
Biogeosciences, 19, 2059–2078, https://doi.org/10.5194/bg-19-2059-2022, https://doi.org/10.5194/bg-19-2059-2022, 2022
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This study tested combinations of two sources of AGB data and two sources of LCC data and used the same burned area satellite data to estimate BB CO emissions. Our analysis showed large discrepancies in annual mean CO emissions and explicit differences in the simulated CO concentrations among the BB emissions estimates. This study has confirmed that BB emissions estimates are sensitive to the land surface information on which they are based.
Johannes Gensheimer, Alexander J. Turner, Philipp Köhler, Christian Frankenberg, and Jia Chen
Biogeosciences, 19, 1777–1793, https://doi.org/10.5194/bg-19-1777-2022, https://doi.org/10.5194/bg-19-1777-2022, 2022
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We develop a convolutional neural network, named SIFnet, that increases the spatial resolution of SIF from TROPOMI by a factor of 10 to a spatial resolution of 0.005°. SIFnet utilizes coarse SIF observations, together with a broad range of high-resolution auxiliary data. The insights gained from interpretable machine learning techniques allow us to make quantitative claims about the relationships between SIF and other common parameters related to photosynthesis.
Shihan Sun, Amos P. K. Tai, David H. Y. Yung, Anthony Y. H. Wong, Jason A. Ducker, and Christopher D. Holmes
Biogeosciences, 19, 1753–1776, https://doi.org/10.5194/bg-19-1753-2022, https://doi.org/10.5194/bg-19-1753-2022, 2022
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We developed and used a terrestrial biosphere model to compare and evaluate widely used empirical dry deposition schemes with different stomatal approaches and found that using photosynthesis-based stomatal approaches can reduce biases in modeled dry deposition velocities in current chemical transport models. Our study shows systematic errors in current dry deposition schemes and the importance of representing plant ecophysiological processes in models under a changing climate.
Ka Ming Fung, Maria Val Martin, and Amos P. K. Tai
Biogeosciences, 19, 1635–1655, https://doi.org/10.5194/bg-19-1635-2022, https://doi.org/10.5194/bg-19-1635-2022, 2022
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Fertilizer-induced ammonia detrimentally affects the environment by not only directly damaging ecosystems but also indirectly altering climate and soil fertility. To quantify these secondary impacts, we enabled CESM to simulate ammonia emission, chemical evolution, and deposition as a continuous cycle. If synthetic fertilizer use is to soar by 30 % from today's level, we showed that the counteracting impacts will increase the global ammonia emission by 3.3 Tg N per year.
Lena Wohlgemuth, Pasi Rautio, Bernd Ahrends, Alexander Russ, Lars Vesterdal, Peter Waldner, Volkmar Timmermann, Nadine Eickenscheidt, Alfred Fürst, Martin Greve, Peter Roskams, Anne Thimonier, Manuel Nicolas, Anna Kowalska, Morten Ingerslev, Päivi Merilä, Sue Benham, Carmen Iacoban, Günter Hoch, Christine Alewell, and Martin Jiskra
Biogeosciences, 19, 1335–1353, https://doi.org/10.5194/bg-19-1335-2022, https://doi.org/10.5194/bg-19-1335-2022, 2022
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Gaseous mercury is present in the atmosphere all over the globe. During the growing season, plants take up mercury from the air in a similar way as CO2. We investigated which factors impact this vegetational mercury uptake by analyzing a large dataset of leaf mercury uptake rates of trees in Europe. As a result, we conclude that mercury uptake is foremost controlled by tree-intrinsic traits like physiological activity but also by climatic factors like dry conditions in the air and in soils.
Junqi Wei, Xiaoyan Li, Lei Liu, Torben Røjle Christensen, Zhiyun Jiang, Yujun Ma, Xiuchen Wu, Hongyun Yao, and Efrén López-Blanco
Biogeosciences, 19, 861–875, https://doi.org/10.5194/bg-19-861-2022, https://doi.org/10.5194/bg-19-861-2022, 2022
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Although water availability has been linked to the response of ecosystem carbon (C) sink–source to climate warming, the mechanisms by which C uptake responds to soil moisture remain unclear. We explored how soil water and other environmental drivers modulate net C uptake in an alpine swamp meadow. Results reveal that nearly saturated soil conditions during warm seasons can help to maintain lower ecosystem respiration and therefore enhance the C sequestration capacity in this alpine swamp meadow.
Martijn M. T. A. Pallandt, Jitendra Kumar, Marguerite Mauritz, Edward A. G. Schuur, Anna-Maria Virkkala, Gerardo Celis, Forrest M. Hoffman, and Mathias Göckede
Biogeosciences, 19, 559–583, https://doi.org/10.5194/bg-19-559-2022, https://doi.org/10.5194/bg-19-559-2022, 2022
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Thawing of Arctic permafrost soils could trigger the release of vast amounts of carbon to the atmosphere, thus enhancing climate change. Our study investigated how well the current network of eddy covariance sites to monitor greenhouse gas exchange at local scales captures pan-Arctic flux patterns. We identified large coverage gaps, e.g., in Siberia, but also demonstrated that a targeted addition of relatively few sites can significantly improve network performance.
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