Articles | Volume 17, issue 12
https://doi.org/10.5194/acp-17-7581-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-17-7581-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
22 Jun 2017
Research article |
| 22 Jun 2017
Nucleation modeling of the Antarctic stratospheric CN layer and derivation of sulfuric acid profiles
Institute for Atmospheric and Environmental Sciences, Goethe
University Frankfurt am Main, 60323 Frankfurt am Main, Germany
now at: Institute for Atmospheric and Climate Science, ETH
Zurich, 8092 Zurich, Switzerland
Joachim Curtius
Institute for Atmospheric and Environmental Sciences, Goethe
University Frankfurt am Main, 60323 Frankfurt am Main, Germany
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Atmos. Chem. Phys., 17, 4871–4885, https://doi.org/10.5194/acp-17-4871-2017, https://doi.org/10.5194/acp-17-4871-2017, 2017
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New particle formation (NPF) is an important atmospheric process. At cold temperatures in the upper troposphere the binary (H2SO4-H2O) and ternary (H2SO4-H2O-NH3) system are thought to be important for NPF. Sulfuric acid monomer (H2SO4) and sulfuric acid dimer ((H2SO4)2) concentrations were measured between 208 and 248K for these systems and dimer evaporation rates were derived. These data will help to better understand and predict binary and ternary nucleation at low temperatures.
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Ice nucleating particles (INP) are important for cloud formation and properties influencing weather and climate. This article presents a method coupling an offline ice nucleus counter to an electron microscope to gain information not only about INP number concentrations but also on important features (size, shape and chemical composition) relevant to ice nucleation on single particles. The method was evaluated on the basis of a case study at the high-altitude research station Jungfraujoch.
Dandan Li, Dongyu Wang, Lucia Caudillo, Wiebke Scholz, Mingyi Wang, Sophie Tomaz, Guillaume Marie, Mihnea Surdu, Elias Eccli, Xianda Gong, Loic Gonzalez-Carracedo, Manuel Granzin, Joschka Pfeifer, Birte Rörup, Benjamin Schulze, Pekka Rantala, Sébastien Perrier, Armin Hansel, Joachim Curtius, Jasper Kirkby, Neil M. Donahue, Christian George, Imad El-Haddad, and Matthieu Riva
Atmos. Meas. Tech., 17, 5413–5428, https://doi.org/10.5194/amt-17-5413-2024, https://doi.org/10.5194/amt-17-5413-2024, 2024
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Due to the analytical challenges of measuring organic vapors, it remains challenging to identify and quantify organic molecules present in the atmosphere. Here, we explore the performance of the Orbitrap chemical ionization mass spectrometer (CI-Orbitrap) using ammonium ion chemistry. This study shows that ammonium-ion-based chemistry associated with the high mass resolution of the Orbitrap mass analyzer can measure almost all inclusive compounds.
Joschka Pfeifer, Naser G. A. Mahfouz, Benjamin C. Schulze, Serge Mathot, Dominik Stolzenburg, Rima Baalbaki, Zoé Brasseur, Lucia Caudillo, Lubna Dada, Manuel Granzin, Xu-Cheng He, Houssni Lamkaddam, Brandon Lopez, Vladimir Makhmutov, Ruby Marten, Bernhard Mentler, Tatjana Müller, Antti Onnela, Maxim Philippov, Ana A. Piedehierro, Birte Rörup, Meredith Schervish, Ping Tian, Nsikanabasi S. Umo, Dongyu S. Wang, Mingyi Wang, Stefan K. Weber, André Welti, Yusheng Wu, Marcel Zauner-Wieczorek, Antonio Amorim, Imad El Haddad, Markku Kulmala, Katrianne Lehtipalo, Tuukka Petäjä, António Tomé, Sander Mirme, Hanna E. Manninen, Neil M. Donahue, Richard C. Flagan, Andreas Kürten, Joachim Curtius, and Jasper Kirkby
Atmos. Chem. Phys., 23, 6703–6718, https://doi.org/10.5194/acp-23-6703-2023, https://doi.org/10.5194/acp-23-6703-2023, 2023
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Attachment rate coefficients between ions and charged aerosol particles determine their lifetimes and may also influence cloud dynamics and aerosol processing. Here we present novel experiments that measure ion–aerosol attachment rate coefficients for multiply charged aerosol particles under atmospheric conditions in the CERN CLOUD chamber. Our results provide experimental discrimination between various theoretical models.
Lucía Caudillo, Mihnea Surdu, Brandon Lopez, Mingyi Wang, Markus Thoma, Steffen Bräkling, Angela Buchholz, Mario Simon, Andrea C. Wagner, Tatjana Müller, Manuel Granzin, Martin Heinritzi, Antonio Amorim, David M. Bell, Zoé Brasseur, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Xu-Cheng He, Houssni Lamkaddam, Naser G. A. Mahfouz, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Roy L. Mauldin, Bernhard Mentler, Antti Onnela, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Birte Rörup, Wiebke Scholz, Jiali Shen, Dominik Stolzenburg, Christian Tauber, Ping Tian, António Tomé, Nsikanabasi Silas Umo, Dongyu S. Wang, Yonghong Wang, Stefan K. Weber, André Welti, Marcel Zauner-Wieczorek, Urs Baltensperger, Richard C. Flagan, Armin Hansel, Jasper Kirkby, Markku Kulmala, Katrianne Lehtipalo, Douglas R. Worsnop, Imad El Haddad, Neil M. Donahue, Alexander L. Vogel, Andreas Kürten, and Joachim Curtius
Atmos. Chem. Phys., 23, 6613–6631, https://doi.org/10.5194/acp-23-6613-2023, https://doi.org/10.5194/acp-23-6613-2023, 2023
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In this study, we present an intercomparison of four different techniques for measuring the chemical composition of nanoparticles. The intercomparison was performed based on the observed chemical composition, calculated volatility, and analysis of the thermograms. We found that the methods generally agree on the most important compounds that are found in the nanoparticles. However, they do see different parts of the organic spectrum. We suggest potential explanations for these differences.
Marcel Zauner-Wieczorek, Joachim Curtius, and Andreas Kürten
Atmos. Chem. Phys., 22, 12443–12465, https://doi.org/10.5194/acp-22-12443-2022, https://doi.org/10.5194/acp-22-12443-2022, 2022
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We reviewed different theories of the ion–ion recombination coefficient α, which describes the reaction and mutual neutralisation of two oppositely charged ions. We focussed on temperature and pressure dependencies and the atmospheric altitude range between 0–50 km. We compared the theories for atmospheric conditions and identified the most favourable value for standard conditions, 1.7 × 10−6 cm3 s−1, and recommend different theories or parameterisations depending on the altitude.
Marcel Zauner-Wieczorek, Martin Heinritzi, Manuel Granzin, Timo Keber, Andreas Kürten, Katharina Kaiser, Johannes Schneider, and Joachim Curtius
Atmos. Chem. Phys., 22, 11781–11794, https://doi.org/10.5194/acp-22-11781-2022, https://doi.org/10.5194/acp-22-11781-2022, 2022
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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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Lucía Caudillo, Birte Rörup, Martin Heinritzi, Guillaume Marie, Mario Simon, Andrea C. Wagner, Tatjana Müller, Manuel Granzin, Antonio Amorim, Farnoush Ataei, Rima Baalbaki, Barbara Bertozzi, Zoé Brasseur, Randall Chiu, Biwu Chu, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Loïc Gonzalez Carracedo, Xu-Cheng He, Victoria Hofbauer, Weimeng Kong, Houssni Lamkaddam, Chuan P. Lee, Brandon Lopez, Naser G. A. Mahfouz, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Dario Massabò, Roy L. Mauldin, Bernhard Mentler, Ugo Molteni, Antti Onnela, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Meredith Schervish, Wiebke Scholz, Benjamin Schulze, Jiali Shen, Dominik Stolzenburg, Yuri Stozhkov, Mihnea Surdu, Christian Tauber, Yee Jun Tham, Ping Tian, António Tomé, Steffen Vogt, Mingyi Wang, Dongyu S. Wang, Stefan K. Weber, André Welti, Wang Yonghong, Wu Yusheng, Marcel Zauner-Wieczorek, Urs Baltensperger, Imad El Haddad, Richard C. Flagan, Armin Hansel, Kristina Höhler, Jasper Kirkby, Markku Kulmala, Katrianne Lehtipalo, Ottmar Möhler, Harald Saathoff, Rainer Volkamer, Paul M. Winkler, Neil M. Donahue, Andreas Kürten, and Joachim Curtius
Atmos. Chem. Phys., 21, 17099–17114, https://doi.org/10.5194/acp-21-17099-2021, https://doi.org/10.5194/acp-21-17099-2021, 2021
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We performed experiments in the CLOUD chamber at CERN at low temperatures to simulate new particle formation in the upper free troposphere (at −30 ºC and −50 ºC). We measured the particle and gas phase and found that most of the compounds present in the gas phase are detected as well in the particle phase. The major compounds in the particles are C8–10 and C18–20. Specifically, we showed that C5 and C15 compounds are detected in a mixed system with isoprene and α-pinene at −30 ºC, 20 % RH.
Mao Xiao, Christopher R. Hoyle, Lubna Dada, Dominik Stolzenburg, Andreas Kürten, Mingyi Wang, Houssni Lamkaddam, Olga Garmash, Bernhard Mentler, Ugo Molteni, Andrea Baccarini, Mario Simon, Xu-Cheng He, Katrianne Lehtipalo, Lauri R. Ahonen, Rima Baalbaki, Paulus S. Bauer, Lisa Beck, David Bell, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, António Dias, Jonathan Duplissy, Henning Finkenzeller, Hamish Gordon, Victoria Hofbauer, Changhyuk Kim, Theodore K. Koenig, Janne Lampilahti, Chuan Ping Lee, Zijun Li, Huajun Mai, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Serge Mathot, Roy L. Mauldin, Wei Nie, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti Rissanen, Siegfried Schobesberger, Simone Schuchmann, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Robert Wagner, Yonghong Wang, Lena Weitz, Daniela Wimmer, Yusheng Wu, Chao Yan, Penglin Ye, Qing Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Ken Carslaw, Joachim Curtius, Armin Hansel, Rainer Volkamer, Paul M. Winkler, Richard C. Flagan, Markku Kulmala, Douglas R. Worsnop, Jasper Kirkby, Neil M. Donahue, Urs Baltensperger, Imad El Haddad, and Josef Dommen
Atmos. Chem. Phys., 21, 14275–14291, https://doi.org/10.5194/acp-21-14275-2021, https://doi.org/10.5194/acp-21-14275-2021, 2021
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Experiments at CLOUD show that in polluted environments new particle formation (NPF) is largely driven by the formation of sulfuric acid–base clusters, stabilized by amines, high ammonia concentrations or lower temperatures. While oxidation products of aromatics can nucleate, they play a minor role in urban NPF. Our experiments span 4 orders of magnitude variation of observed NPF rates in ambient conditions. We provide a framework based on NPF and growth rates to interpret ambient observations.
Mingyi Wang, Xu-Cheng He, Henning Finkenzeller, Siddharth Iyer, Dexian Chen, Jiali Shen, Mario Simon, Victoria Hofbauer, Jasper Kirkby, Joachim Curtius, Norbert Maier, Theo Kurtén, Douglas R. Worsnop, Markku Kulmala, Matti Rissanen, Rainer Volkamer, Yee Jun Tham, Neil M. Donahue, and Mikko Sipilä
Atmos. Meas. Tech., 14, 4187–4202, https://doi.org/10.5194/amt-14-4187-2021, https://doi.org/10.5194/amt-14-4187-2021, 2021
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Atmospheric iodine species are often short-lived with low abundance and have thus been challenging to measure. We show that the bromide chemical ionization mass spectrometry, compatible with both the atmospheric pressure and reduced pressure interfaces, can simultaneously detect various gas-phase iodine species. Combining calibration experiments and quantum chemical calculations, we quantify detection sensitivities to HOI, HIO3, I2, and H2SO4, giving detection limits down to < 106 molec. cm-3.
Jann Schrod, Erik S. Thomson, Daniel Weber, Jens Kossmann, Christopher Pöhlker, Jorge Saturno, Florian Ditas, Paulo Artaxo, Valérie Clouard, Jean-Marie Saurel, Martin Ebert, Joachim Curtius, and Heinz G. Bingemer
Atmos. Chem. Phys., 20, 15983–16006, https://doi.org/10.5194/acp-20-15983-2020, https://doi.org/10.5194/acp-20-15983-2020, 2020
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Long-term ice-nucleating particle (INP) data are presented from four semi-pristine sites located in the Amazon, the Caribbean, Germany and the Arctic. Average INP concentrations did not differ by orders of magnitude between the sites. For all sites short-term variability dominated the time series, which lacked clear trends and seasonalities. Common drivers to explain the INP levels and their variations could not be identified, illustrating the complex nature of heterogeneous ice nucleation.
Jann Schrod, Dominik Kleinhenz, Maria Hörhold, Tobias Erhardt, Sarah Richter, Frank Wilhelms, Hubertus Fischer, Martin Ebert, Birthe Twarloh, Damiano Della Lunga, Camilla M. Jensen, Joachim Curtius, and Heinz G. Bingemer
Atmos. Chem. Phys., 20, 12459–12482, https://doi.org/10.5194/acp-20-12459-2020, https://doi.org/10.5194/acp-20-12459-2020, 2020
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Ice-nucleating particle (INP) concentrations of the last 6 centuries are presented from an ice core in Greenland. The data are accompanied by physical and chemical aerosol data. INPs are correlated to the dust signal from the ice core and seem to follow the annual input of mineral dust. We find no clear trend in the INP concentration. However, modern-day concentrations are higher and more variable than the concentrations of the past. This might have significant atmospheric implications.
Martin Heinritzi, Lubna Dada, Mario Simon, Dominik Stolzenburg, Andrea C. Wagner, Lukas Fischer, Lauri R. Ahonen, Stavros Amanatidis, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Bernhard Baumgartner, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, Antonio Dias, Josef Dommen, Jonathan Duplissy, Henning Finkenzeller, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Manuel Granzin, Imad El Haddad, Xucheng He, Johanna Helm, Victoria Hofbauer, Christopher R. Hoyle, Juha Kangasluoma, Timo Keber, Changhyuk Kim, Andreas Kürten, Houssni Lamkaddam, Tiia M. Laurila, Janne Lampilahti, Chuan Ping Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Vladimir Makhmutov, Hanna Elina Manninen, Ruby Marten, Serge Mathot, Roy Lee Mauldin, Bernhard Mentler, Ugo Molteni, Tatjana Müller, Wei Nie, Tuomo Nieminen, Antti Onnela, Eva Partoll, Monica Passananti, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti P. Rissanen, Clémence Rose, Siegfried Schobesberger, Wiebke Scholz, Kay Scholze, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, Miguel Vazquez-Pufleau, Annele Virtanen, Alexander L. Vogel, Rainer Volkamer, Robert Wagner, Mingyi Wang, Lena Weitz, Daniela Wimmer, Mao Xiao, Chao Yan, Penglin Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Urs Baltensperger, Armin Hansel, Markku Kulmala, António Tomé, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 11809–11821, https://doi.org/10.5194/acp-20-11809-2020, https://doi.org/10.5194/acp-20-11809-2020, 2020
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With experiments performed at CLOUD, we show how isoprene interferes in monoterpene oxidation via RO2 termination at atmospherically relevant concentrations. This interference shifts the distribution of highly oxygenated organic molecules (HOMs) away from C20 class dimers towards C15 class dimers, which subsequently reduces both biogenic nucleation and early growth rates. Our results may help to understand the absence of new-particle formation in isoprene-rich environments.
Mario Simon, Lubna Dada, Martin Heinritzi, Wiebke Scholz, Dominik Stolzenburg, Lukas Fischer, Andrea C. Wagner, Andreas Kürten, Birte Rörup, Xu-Cheng He, João Almeida, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Lisa Beck, Anton Bergen, Federico Bianchi, Steffen Bräkling, Sophia Brilke, Lucia Caudillo, Dexian Chen, Biwu Chu, António Dias, Danielle C. Draper, Jonathan Duplissy, Imad El-Haddad, Henning Finkenzeller, Carla Frege, Loic Gonzalez-Carracedo, Hamish Gordon, Manuel Granzin, Jani Hakala, Victoria Hofbauer, Christopher R. Hoyle, Changhyuk Kim, Weimeng Kong, Houssni Lamkaddam, Chuan P. Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Bernhard Mentler, Ugo Molteni, Leonid Nichman, Wei Nie, Andrea Ojdanic, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Lauriane L. J. Quéléver, Ananth Ranjithkumar, Matti P. Rissanen, Simon Schallhart, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee J. Tham, António R. Tomé, Miguel Vazquez-Pufleau, Alexander L. Vogel, Robert Wagner, Mingyi Wang, Dongyu S. Wang, Yonghong Wang, Stefan K. Weber, Yusheng Wu, Mao Xiao, Chao Yan, Penglin Ye, Qing Ye, Marcel Zauner-Wieczorek, Xueqin Zhou, Urs Baltensperger, Josef Dommen, Richard C. Flagan, Armin Hansel, Markku Kulmala, Rainer Volkamer, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 9183–9207, https://doi.org/10.5194/acp-20-9183-2020, https://doi.org/10.5194/acp-20-9183-2020, 2020
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Highly oxygenated organic compounds (HOMs) have been identified as key vapors involved in atmospheric new-particle formation (NPF). The molecular distribution, HOM yield, and NPF from α-pinene oxidation experiments were measured at the CLOUD chamber over a wide tropospheric-temperature range. This study shows on a molecular scale that despite the sharp reduction in HOM yield at lower temperatures, the reduced volatility counteracts this effect and leads to an overall increase in the NPF rate.
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.
Joschka Pfeifer, Mario Simon, Martin Heinritzi, Felix Piel, Lena Weitz, Dongyu Wang, Manuel Granzin, Tatjana Müller, Steffen Bräkling, Jasper Kirkby, Joachim Curtius, and Andreas Kürten
Atmos. Meas. Tech., 13, 2501–2522, https://doi.org/10.5194/amt-13-2501-2020, https://doi.org/10.5194/amt-13-2501-2020, 2020
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Ammonia is an important atmospheric trace gas that affects secondary aerosol formation and, together with sulfuric acid, the formation of new particles. A measurement technique is presented that uses high-resolution mass spectrometry and protonated water clusters for the ultrasensitive detection of ammonia at single-digit parts per trillion by volume levels. The instrument is further capable of measuring amines and a suite of iodine compounds at sub-parts per trillion by volume levels.
Naruki Hiranuma, Kouji Adachi, David M. Bell, Franco Belosi, Hassan Beydoun, Bhaskar Bhaduri, Heinz Bingemer, Carsten Budke, Hans-Christian Clemen, Franz Conen, Kimberly M. Cory, Joachim Curtius, Paul J. DeMott, Oliver Eppers, Sarah Grawe, Susan Hartmann, Nadine Hoffmann, Kristina Höhler, Evelyn Jantsch, Alexei Kiselev, Thomas Koop, Gourihar Kulkarni, Amelie Mayer, Masataka Murakami, Benjamin J. Murray, Alessia Nicosia, Markus D. Petters, Matteo Piazza, Michael Polen, Naama Reicher, Yinon Rudich, Atsushi Saito, Gianni Santachiara, Thea Schiebel, Gregg P. Schill, Johannes Schneider, Lior Segev, Emiliano Stopelli, Ryan C. Sullivan, Kaitlyn Suski, Miklós Szakáll, Takuya Tajiri, Hans Taylor, Yutaka Tobo, Romy Ullrich, Daniel Weber, Heike Wex, Thomas F. Whale, Craig L. Whiteside, Katsuya Yamashita, Alla Zelenyuk, and Ottmar Möhler
Atmos. Chem. Phys., 19, 4823–4849, https://doi.org/10.5194/acp-19-4823-2019, https://doi.org/10.5194/acp-19-4823-2019, 2019
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A total of 20 ice nucleation measurement techniques contributed to investigate the immersion freezing behavior of cellulose particles – natural polymers. Our data showed several types of cellulose are able to nucleate ice as efficiently as some mineral dust samples and cellulose has the potential to be an important atmospheric ice-nucleating particle. Continued investigation/collaboration is necessary to obtain further insight into consistency or diversity of ice nucleation measurements.
Andrea C. Wagner, Anton Bergen, Sophia Brilke, Claudia Fuchs, Markus Ernst, Jesica Hoker, Martin Heinritzi, Mario Simon, Bertram Bühner, Joachim Curtius, and Andreas Kürten
Atmos. Meas. Tech., 11, 5489–5506, https://doi.org/10.5194/amt-11-5489-2018, https://doi.org/10.5194/amt-11-5489-2018, 2018
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Chemical analysis of sub-30 nm aerosol particles is important for understanding aerosol nucleation and early growth, yet it is still an experimental challenge. In this study, we present a novel device for size resolved chemical analysis of nucleation and Aitken mode particles (from ~10 to ~30 nm) while allowing gas phase measurements with the same detector. Particles are charged, size selected, electrostatically collected and then thermally desorbed in a carrier gas.
Nina Sarnela, Tuija Jokinen, Jonathan Duplissy, Chao Yan, Tuomo Nieminen, Mikael Ehn, Siegfried Schobesberger, Martin Heinritzi, Sebastian Ehrhart, Katrianne Lehtipalo, Jasmin Tröstl, Mario Simon, Andreas Kürten, Markus Leiminger, Michael J. Lawler, Matti P. Rissanen, Federico Bianchi, Arnaud P. Praplan, Jani Hakala, Antonio Amorim, Marc Gonin, Armin Hansel, Jasper Kirkby, Josef Dommen, Joachim Curtius, James N. Smith, Tuukka Petäjä, Douglas R. Worsnop, Markku Kulmala, Neil M. Donahue, and Mikko Sipilä
Atmos. Chem. Phys., 18, 2363–2380, https://doi.org/10.5194/acp-18-2363-2018, https://doi.org/10.5194/acp-18-2363-2018, 2018
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Atmospheric trace gases can form small molecular clusters, which can grow to larger sizes through the condensation of vapours. This process is called new particle formation. In this paper we studied the formation of sulfuric acid and highly oxygenated molecules, the key compounds in atmospheric new particle formation, in chamber experiments and introduced a way to simulate these ozonolysis products of α-pinene in a simple manner.
Andreas Kürten, Chenxi Li, Federico Bianchi, Joachim Curtius, António Dias, Neil M. Donahue, Jonathan Duplissy, Richard C. Flagan, Jani Hakala, Tuija Jokinen, Jasper Kirkby, Markku Kulmala, Ari Laaksonen, Katrianne Lehtipalo, Vladimir Makhmutov, Antti Onnela, Matti P. Rissanen, Mario Simon, Mikko Sipilä, Yuri Stozhkov, Jasmin Tröstl, Penglin Ye, and Peter H. McMurry
Atmos. Chem. Phys., 18, 845–863, https://doi.org/10.5194/acp-18-845-2018, https://doi.org/10.5194/acp-18-845-2018, 2018
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A recent laboratory study (CLOUD) showed that new particles nucleate efficiently from sulfuric acid and dimethylamine (DMA). The reanalysis of previously published data reveals that the nucleation rates are even faster than previously assumed, i.e., nucleation can proceed at rates that are compatible with collision-controlled new particle formation for atmospheric conditions. This indicates that sulfuric acid–DMA nucleation is likely an important source of particles in the boundary layer.
Carla Frege, Ismael K. Ortega, Matti P. Rissanen, Arnaud P. Praplan, Gerhard Steiner, Martin Heinritzi, Lauri Ahonen, António Amorim, Anne-Kathrin Bernhammer, Federico Bianchi, Sophia Brilke, Martin Breitenlechner, Lubna Dada, António Dias, Jonathan Duplissy, Sebastian Ehrhart, Imad El-Haddad, Lukas Fischer, Claudia Fuchs, Olga Garmash, Marc Gonin, Armin Hansel, Christopher R. Hoyle, Tuija Jokinen, Heikki Junninen, Jasper Kirkby, Andreas Kürten, Katrianne Lehtipalo, Markus Leiminger, Roy Lee Mauldin, Ugo Molteni, Leonid Nichman, Tuukka Petäjä, Nina Sarnela, Siegfried Schobesberger, Mario Simon, Mikko Sipilä, Dominik Stolzenburg, António Tomé, Alexander L. Vogel, Andrea C. Wagner, Robert Wagner, Mao Xiao, Chao Yan, Penglin Ye, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Markku Kulmala, Douglas R. Worsnop, Paul M. Winkler, Josef Dommen, and Urs Baltensperger
Atmos. Chem. Phys., 18, 65–79, https://doi.org/10.5194/acp-18-65-2018, https://doi.org/10.5194/acp-18-65-2018, 2018
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It was recently shown that biogenic highly oxygenated molecules (HOMs) form particles in the absence of sulfuric acid and ions enhance the nucleation rate. Here we compare the molecular composition of positive and negative HOM clusters at 25, 5 and −25 °C. At lower temperatures the HOM average oxygen-to-carbon ratio decreases indicating a reduction in the rate of autoxidation due to rather high activation energy. The experimental findings are supported by quantum chemical calculations.
Robert Wagner, Chao Yan, Katrianne Lehtipalo, Jonathan Duplissy, Tuomo Nieminen, Juha Kangasluoma, Lauri R. Ahonen, Lubna Dada, Jenni Kontkanen, Hanna E. Manninen, Antonio Dias, Antonio Amorim, Paulus S. Bauer, Anton Bergen, Anne-Kathrin Bernhammer, Federico Bianchi, Sophia Brilke, Stephany Buenrostro Mazon, Xuemeng Chen, Danielle C. Draper, Lukas Fischer, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Jani Hakala, Liine Heikkinen, Martin Heinritzi, Victoria Hofbauer, Christopher R. Hoyle, Jasper Kirkby, Andreas Kürten, Alexander N. Kvashnin, Tiia Laurila, Michael J. Lawler, Huajun Mai, Vladimir Makhmutov, Roy L. Mauldin III, Ugo Molteni, Leonid Nichman, Wei Nie, Andrea Ojdanic, Antti Onnela, Felix Piel, Lauriane L. J. Quéléver, Matti P. Rissanen, Nina Sarnela, Simon Schallhart, Kamalika Sengupta, Mario Simon, Dominik Stolzenburg, Yuri Stozhkov, Jasmin Tröstl, Yrjö Viisanen, Alexander L. Vogel, Andrea C. Wagner, Mao Xiao, Penglin Ye, Urs Baltensperger, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Martin Gallagher, Armin Hansel, James N. Smith, António Tomé, Paul M. Winkler, Douglas Worsnop, Mikael Ehn, Mikko Sipilä, Veli-Matti Kerminen, Tuukka Petäjä, and Markku Kulmala
Atmos. Chem. Phys., 17, 15181–15197, https://doi.org/10.5194/acp-17-15181-2017, https://doi.org/10.5194/acp-17-15181-2017, 2017
Georgios Tsagkogeorgas, Pontus Roldin, Jonathan Duplissy, Linda Rondo, Jasmin Tröstl, Jay G. Slowik, Sebastian Ehrhart, Alessandro Franchin, Andreas Kürten, Antonio Amorim, Federico Bianchi, Jasper Kirkby, Tuukka Petäjä, Urs Baltensperger, Michael Boy, Joachim Curtius, Richard C. Flagan, Markku Kulmala, Neil M. Donahue, and Frank Stratmann
Atmos. Chem. Phys., 17, 8923–8938, https://doi.org/10.5194/acp-17-8923-2017, https://doi.org/10.5194/acp-17-8923-2017, 2017
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The H2SO4 vapour pressure plays key role in Earth's and Venus' atmospheres. In regions where RH is low and stabilising bases are scarce, H2SO4 can evaporate from particles; however the H2SO4 vapour pressure at low RH is uncertain. To address this, we measured H2SO4 evaporation versus T and RH in the CLOUD chamber and constrained the equilibrium constants for dissociation and dehydration of H2SO4. This study is important for nucleation, particle growth and H2SO4 formation occurring in atmosphere.
Blaž Gasparini, Steffen Münch, Laure Poncet, Monika Feldmann, and Ulrike Lohmann
Atmos. Chem. Phys., 17, 4871–4885, https://doi.org/10.5194/acp-17-4871-2017, https://doi.org/10.5194/acp-17-4871-2017, 2017
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Cirrus clouds have, unlike other cloud types, a warming impact on climate. Decreasing their frequency therefore leads to a cooling effect. Cirrus ice crystals grow larger when formed on solid aerosols, inducing a shorter cloud lifetime.
We compare simplified simulations of stripping cirrus out of the sky with simulations of seeding by aerosol injections. While we find the surface climate responses to be similar, the changes in clouds and cloud properties differ significantly.
Jann Schrod, Daniel Weber, Jaqueline Drücke, Christos Keleshis, Michael Pikridas, Martin Ebert, Bojan Cvetković, Slobodan Nickovic, Eleni Marinou, Holger Baars, Albert Ansmann, Mihalis Vrekoussis, Nikos Mihalopoulos, Jean Sciare, Joachim Curtius, and Heinz G. Bingemer
Atmos. Chem. Phys., 17, 4817–4835, https://doi.org/10.5194/acp-17-4817-2017, https://doi.org/10.5194/acp-17-4817-2017, 2017
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In this paper we present data of ice-nucleating particles (INPs) from a 1-month campaign in the Eastern Mediterranean using unmanned aircraft systems (UASs, drones) and offline sampling with subsequent laboratory analysis. To our knowledge, this is the first time INPs were measured onboard a UAS. We find that INP concentrations were 1 magnitude higher aloft than at the ground, highlighting that surface-based measurement of INP may only be of limited significance for the situation at cloud level.
Susan Schmidt, Johannes Schneider, Thomas Klimach, Stephan Mertes, Ludwig Paul Schenk, Piotr Kupiszewski, Joachim Curtius, and Stephan Borrmann
Atmos. Chem. Phys., 17, 575–594, https://doi.org/10.5194/acp-17-575-2017, https://doi.org/10.5194/acp-17-575-2017, 2017
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Ice formation in clouds is an important process in the formation of precipitation, especially at midlatitudes, but the exact properties of the aerosol particles that initiate freezing is not fully understood. We analysed residual particles from ice crystals sampled from mixed phase clouds. The results show that the residues contain a larger relative amount of soil dust and minerals, but also particles from industrial emissions and lead-containing particles, than the out-of-cloud aerosol.
Andreas Kürten, Anton Bergen, Martin Heinritzi, Markus Leiminger, Verena Lorenz, Felix Piel, Mario Simon, Robert Sitals, Andrea C. Wagner, and Joachim Curtius
Atmos. Chem. Phys., 16, 12793–12813, https://doi.org/10.5194/acp-16-12793-2016, https://doi.org/10.5194/acp-16-12793-2016, 2016
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Field measurements were conducted at a rural site in central Germany close to dairy farms to investigate if there is a connection between new particle formation and the presence of amines. A variety of trace gases were measured in addition to amines, like sulfuric acid, ammonia and highly oxygenated organic molecules (HOM). The results indicate that amines are very likely involved in the growth of aerosol particles and probably also in the nucleation process, although HOM could be relevant, too.
Karoliina Ignatius, Thomas B. Kristensen, Emma Järvinen, Leonid Nichman, Claudia Fuchs, Hamish Gordon, Paul Herenz, Christopher R. Hoyle, Jonathan Duplissy, Sarvesh Garimella, Antonio Dias, Carla Frege, Niko Höppel, Jasmin Tröstl, Robert Wagner, Chao Yan, Antonio Amorim, Urs Baltensperger, Joachim Curtius, Neil M. Donahue, Martin W. Gallagher, Jasper Kirkby, Markku Kulmala, Ottmar Möhler, Harald Saathoff, Martin Schnaiter, Antonio Tomé, Annele Virtanen, Douglas Worsnop, and Frank Stratmann
Atmos. Chem. Phys., 16, 6495–6509, https://doi.org/10.5194/acp-16-6495-2016, https://doi.org/10.5194/acp-16-6495-2016, 2016
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Viscous solid or semi-solid secondary organic aerosol (SOA) may influence cloud properties through ice nucleation in the atmosphere. Here, we observed heterogeneous ice nucleation of viscous α-pinene SOA at temperatures between −39 °C and −37.2 °C with ice saturation ratios significantly below the homogeneous freezing limit. Global modelling suggests that viscous biogenic SOA are present in regions where cirrus formation takes place and could contribute to the global ice nuclei budget.
Mario Simon, Martin Heinritzi, Stephan Herzog, Markus Leiminger, Federico Bianchi, Arnaud Praplan, Josef Dommen, Joachim Curtius, and Andreas Kürten
Atmos. Meas. Tech., 9, 2135–2145, https://doi.org/10.5194/amt-9-2135-2016, https://doi.org/10.5194/amt-9-2135-2016, 2016
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This study demonstrate the detection of dimethylamine at low mixing ratios by nitrate chemical ionization mass spectrometry (CIMS). Due to simultaneously high-sensitive gas-phase measurements of DMA, sulfuric acid, and extremely low volatile organic compounds (ELVOCs), this technique can be used as a versatile tool for studying new particle formation in the atmosphere.
Martin Heinritzi, Mario Simon, Gerhard Steiner, Andrea C. Wagner, Andreas Kürten, Armin Hansel, and Joachim Curtius
Atmos. Meas. Tech., 9, 1449–1460, https://doi.org/10.5194/amt-9-1449-2016, https://doi.org/10.5194/amt-9-1449-2016, 2016
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An easy-to-use method of estimating the mass-dependent transmission efficiency of a CIMS is presented. It makes use of depleting nitrate primary ions by different perfluorinated acids to obtain the transmission efficiency of these acids relative to the primary ion. Knowledge about the transmission efficiency is crucial for, e.g., quantification of extremely low volatile organic compounds.
C. R. Hoyle, C. Fuchs, E. Järvinen, H. Saathoff, A. Dias, I. El Haddad, M. Gysel, S. C. Coburn, J. Tröstl, A.-K. Bernhammer, F. Bianchi, M. Breitenlechner, J. C. Corbin, J. Craven, N. M. Donahue, J. Duplissy, S. Ehrhart, C. Frege, H. Gordon, N. Höppel, M. Heinritzi, T. B. Kristensen, U. Molteni, L. Nichman, T. Pinterich, A. S. H. Prévôt, M. Simon, J. G. Slowik, G. Steiner, A. Tomé, A. L. Vogel, R. Volkamer, A. C. Wagner, R. Wagner, A. S. Wexler, C. Williamson, P. M. Winkler, C. Yan, A. Amorim, J. Dommen, J. Curtius, M. W. Gallagher, R. C. Flagan, A. Hansel, J. Kirkby, M. Kulmala, O. Möhler, F. Stratmann, D. R. Worsnop, and U. Baltensperger
Atmos. Chem. Phys., 16, 1693–1712, https://doi.org/10.5194/acp-16-1693-2016, https://doi.org/10.5194/acp-16-1693-2016, 2016
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A significant portion of sulphate, an important constituent of atmospheric aerosols, is formed via the aqueous phase oxidation of sulphur dioxide by ozone. The rate of this reaction has previously only been measured over a relatively small temperature range. Here, we use the state of the art CLOUD chamber at CERN to perform the first measurements of this reaction rate in super-cooled droplets, confirming that the existing extrapolation of the reaction rate to sub-zero temperatures is accurate.
J. Kim, L. Ahlm, T. Yli-Juuti, M. Lawler, H. Keskinen, J. Tröstl, S. Schobesberger, J. Duplissy, A. Amorim, F. Bianchi, N. M. Donahue, R. C. Flagan, J. Hakala, M. Heinritzi, T. Jokinen, A. Kürten, A. Laaksonen, K. Lehtipalo, P. Miettinen, T. Petäjä, M. P. Rissanen, L. Rondo, K. Sengupta, M. Simon, A. Tomé, C. Williamson, D. Wimmer, P. M. Winkler, S. Ehrhart, P. Ye, J. Kirkby, J. Curtius, U. Baltensperger, M. Kulmala, K. E. J. Lehtinen, J. N. Smith, I. Riipinen, and A. Virtanen
Atmos. Chem. Phys., 16, 293–304, https://doi.org/10.5194/acp-16-293-2016, https://doi.org/10.5194/acp-16-293-2016, 2016
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The hygroscopicity of nucleated nanoparticles was measured in the presence of sulfuric acid, sulfuric acid-dimethylamine, and sulfuric acid-organics derived from α-pinene oxidation during CLOUD7 at CERN in 2012. The hygroscopicity parameter κ decreased with increasing particle size, indicating decreasing acidity of particles.
A. Kürten, S. Münch, L. Rondo, F. Bianchi, J. Duplissy, T. Jokinen, H. Junninen, N. Sarnela, S. Schobesberger, M. Simon, M. Sipilä, J. Almeida, A. Amorim, J. Dommen, N. M. Donahue, E. M. Dunne, R. C. Flagan, A. Franchin, J. Kirkby, A. Kupc, V. Makhmutov, T. Petäjä, A. P. Praplan, F. Riccobono, G. Steiner, A. Tomé, G. Tsagkogeorgas, P. E. Wagner, D. Wimmer, U. Baltensperger, M. Kulmala, D. R. Worsnop, and J. Curtius
Atmos. Chem. Phys., 15, 10701–10721, https://doi.org/10.5194/acp-15-10701-2015, https://doi.org/10.5194/acp-15-10701-2015, 2015
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New particle formation (NPF) is an important atmospheric process. At cold temperatures in the upper troposphere the binary (H2SO4-H2O) and ternary (H2SO4-H2O-NH3) system are thought to be important for NPF. Sulfuric acid monomer (H2SO4) and sulfuric acid dimer ((H2SO4)2) concentrations were measured between 208 and 248K for these systems and dimer evaporation rates were derived. These data will help to better understand and predict binary and ternary nucleation at low temperatures.
D. Wimmer, K. Lehtipalo, T. Nieminen, J. Duplissy, S. Ehrhart, J. Almeida, L. Rondo, A. Franchin, F. Kreissl, F. Bianchi, H. E. Manninen, M. Kulmala, J. Curtius, and T. Petäjä
Atmos. Chem. Phys., 15, 7547–7555, https://doi.org/10.5194/acp-15-7547-2015, https://doi.org/10.5194/acp-15-7547-2015, 2015
A. Franchin, S. Ehrhart, J. Leppä, T. Nieminen, S. Gagné, S. Schobesberger, D. Wimmer, J. Duplissy, F. Riccobono, E. M. Dunne, L. Rondo, A. Downard, F. Bianchi, A. Kupc, G. Tsagkogeorgas, K. Lehtipalo, H. E. Manninen, J. Almeida, A. Amorim, P. E. Wagner, A. Hansel, J. Kirkby, A. Kürten, N. M. Donahue, V. Makhmutov, S. Mathot, A. Metzger, T. Petäjä, R. Schnitzhofer, M. Sipilä, Y. Stozhkov, A. Tomé, V.-M. Kerminen, K. Carslaw, J. Curtius, U. Baltensperger, and M. Kulmala
Atmos. Chem. Phys., 15, 7203–7216, https://doi.org/10.5194/acp-15-7203-2015, https://doi.org/10.5194/acp-15-7203-2015, 2015
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The ion-ion recombination coefficient was measured at different temperatures, relative humidities and concentrations of ozone and sulfur dioxide. The experiments were carried out using the CLOUD chamber at CERN.
We observed a strong dependency on temperature and on relative humidity, which has not been reported previously. No dependency of the ion-ion recombination coefficient on ozone concentration was observed and a weak variation with sulfur dioxide concentration was also observed.
A. Worringen, K. Kandler, N. Benker, T. Dirsch, S. Mertes, L. Schenk, U. Kästner, F. Frank, B. Nillius, U. Bundke, D. Rose, J. Curtius, P. Kupiszewski, E. Weingartner, P. Vochezer, J. Schneider, S. Schmidt, S. Weinbruch, and M. Ebert
Atmos. Chem. Phys., 15, 4161–4178, https://doi.org/10.5194/acp-15-4161-2015, https://doi.org/10.5194/acp-15-4161-2015, 2015
A. P. Praplan, S. Schobesberger, F. Bianchi, M. P. Rissanen, M. Ehn, T. Jokinen, H. Junninen, A. Adamov, A. Amorim, J. Dommen, J. Duplissy, J. Hakala, A. Hansel, M. Heinritzi, J. Kangasluoma, J. Kirkby, M. Krapf, A. Kürten, K. Lehtipalo, F. Riccobono, L. Rondo, N. Sarnela, M. Simon, A. Tomé, J. Tröstl, P. M. Winkler, C. Williamson, P. Ye, J. Curtius, U. Baltensperger, N. M. Donahue, M. Kulmala, and D. R. Worsnop
Atmos. Chem. Phys., 15, 4145–4159, https://doi.org/10.5194/acp-15-4145-2015, https://doi.org/10.5194/acp-15-4145-2015, 2015
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Our study shows, based on data from three atmospheric pressure interface time-of-flight mass spectrometers measuring in parallel charged and neutral molecules and molecular clusters, how oxidised organic compounds bind to inorganic ions (e.g. bisulfate, nitrate, ammonium). This ionisation is selective for compounds with lower molar mass due to their limited amount and variety of functional groups. We also found that extremely low volatile organic compounds (ELVOCs) can be formed immediately.
A. Kürten, C. Williamson, J. Almeida, J. Kirkby, and J. Curtius
Atmos. Chem. Phys., 15, 4063–4075, https://doi.org/10.5194/acp-15-4063-2015, https://doi.org/10.5194/acp-15-4063-2015, 2015
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The manuscript provides insights into the calculation of new particle formation rates. Generally, formation rates are measured at a diameter which can be substantially larger than the critical size of the newly formed particles. In order to transform the formation rate to a smaller size, a correction needs to be applied. We present a new method to apply this correction which takes into account the effect of self-coagulation.
N. Hiranuma, S. Augustin-Bauditz, H. Bingemer, C. Budke, J. Curtius, A. Danielczok, K. Diehl, K. Dreischmeier, M. Ebert, F. Frank, N. Hoffmann, K. Kandler, A. Kiselev, T. Koop, T. Leisner, O. Möhler, B. Nillius, A. Peckhaus, D. Rose, S. Weinbruch, H. Wex, Y. Boose, P. J. DeMott, J. D. Hader, T. C. J. Hill, Z. A. Kanji, G. Kulkarni, E. J. T. Levin, C. S. McCluskey, M. Murakami, B. J. Murray, D. Niedermeier, M. D. Petters, D. O'Sullivan, A. Saito, G. P. Schill, T. Tajiri, M. A. Tolbert, A. Welti, T. F. Whale, T. P. Wright, and K. Yamashita
Atmos. Chem. Phys., 15, 2489–2518, https://doi.org/10.5194/acp-15-2489-2015, https://doi.org/10.5194/acp-15-2489-2015, 2015
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Seventeen ice nucleation measurement techniques contributed to investigate the immersion freezing behavior of illite NX. All data showed a similar temperature trend, but the measured ice nucleation activity was on average smaller for the wet suspended samples and higher for the dry-dispersed aerosol samples at high temperatures. A continued investigation and collaboration is necessary to obtain further insights into consistency or diversity of ice nucleation measurements.
S. Schmidt, J. Schneider, T. Klimach, S. Mertes, L. P. Schenk, J. Curtius, P. Kupiszewski, E. Hammer, P. Vochezer, G. Lloyd, M. Ebert, K. Kandler, S. Weinbruch, and S. Borrmann
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-15-4677-2015, https://doi.org/10.5194/acpd-15-4677-2015, 2015
Revised manuscript not accepted
H. Wex, S. Augustin-Bauditz, Y. Boose, C. Budke, J. Curtius, K. Diehl, A. Dreyer, F. Frank, S. Hartmann, N. Hiranuma, E. Jantsch, Z. A. Kanji, A. Kiselev, T. Koop, O. Möhler, D. Niedermeier, B. Nillius, M. Rösch, D. Rose, C. Schmidt, I. Steinke, and F. Stratmann
Atmos. Chem. Phys., 15, 1463–1485, https://doi.org/10.5194/acp-15-1463-2015, https://doi.org/10.5194/acp-15-1463-2015, 2015
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Immersion freezing measurements from seven different measurement techniques were intercompared using a biological ice nucleating material from bacteria. Although different techniques examined differently concentrated droplets, it was possible to find a uniform description, which showed that results from all experiments were generally in good agreement and were also in agreement with parameterizations published earlier in literature.
S. Schobesberger, A. Franchin, F. Bianchi, L. Rondo, J. Duplissy, A. Kürten, I. K. Ortega, A. Metzger, R. Schnitzhofer, J. Almeida, A. Amorim, J. Dommen, E. M. Dunne, M. Ehn, S. Gagné, L. Ickes, H. Junninen, A. Hansel, V.-M. Kerminen, J. Kirkby, A. Kupc, A. Laaksonen, K. Lehtipalo, S. Mathot, A. Onnela, T. Petäjä, F. Riccobono, F. D. Santos, M. Sipilä, A. Tomé, G. Tsagkogeorgas, Y. Viisanen, P. E. Wagner, D. Wimmer, J. Curtius, N. M. Donahue, U. Baltensperger, M. Kulmala, and D. R. Worsnop
Atmos. Chem. Phys., 15, 55–78, https://doi.org/10.5194/acp-15-55-2015, https://doi.org/10.5194/acp-15-55-2015, 2015
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We used an ion mass spectrometer at CERN's CLOUD chamber to investigate the detailed composition of ammonia--sulfuric acid ion clusters (of both polarities) as they initially form and then grow into aerosol particles, at atmospherically relevant conditions. We found that these clusters’ composition is mainly determined by the ratio of the precursor vapors and ranges from ammonia-free clusters to clusters containing > 1 ammonia per sulfuric acid. Acid--base bindings are a key formation mechanism.
L. Rondo, A. Kürten, S. Ehrhart, S. Schobesberger, A. Franchin, H. Junninen, T. Petäjä, M. Sipilä, D. R. Worsnop, and J. Curtius
Atmos. Meas. Tech., 7, 3849–3859, https://doi.org/10.5194/amt-7-3849-2014, https://doi.org/10.5194/amt-7-3849-2014, 2014
L. P. Schenk, S. Mertes, U. Kästner, F. Frank, B. Nillius, U. Bundke, D. Rose, S. Schmidt, J. Schneider, A. Worringen, K. Kandler, N. Bukowiecki, M. Ebert, J. Curtius, and F. Stratmann
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amtd-7-10585-2014, https://doi.org/10.5194/amtd-7-10585-2014, 2014
Revised manuscript has not been submitted
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A pumped counterflow virtual impactor (PCVI) was set up to separate ice nucleating particle (INP) counter produced ice particles that had been activated to ice from non-activated aerosol particles. The released INP were characterized with regard to their physico-chemical properties. A successful separation (PCVI) of INP for water-subsaturated conditions is proven. First results of INP properties are presented which were gained during a campaign at the high altitude research station Jungfraujoch.
D. Rose, S. S. Gunthe, Z. Jurányi, M. Gysel, G. P. Frank, J. Schneider, J. Curtius, and U. Pöschl
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-13-32575-2013, https://doi.org/10.5194/acpd-13-32575-2013, 2013
Revised manuscript has not been submitted
S. Ehrhart and J. Curtius
Atmos. Chem. Phys., 13, 11465–11471, https://doi.org/10.5194/acp-13-11465-2013, https://doi.org/10.5194/acp-13-11465-2013, 2013
H. Keskinen, A. Virtanen, J. Joutsensaari, G. Tsagkogeorgas, J. Duplissy, S. Schobesberger, M. Gysel, F. Riccobono, J. G. Slowik, F. Bianchi, T. Yli-Juuti, K. Lehtipalo, L. Rondo, M. Breitenlechner, A. Kupc, J. Almeida, A. Amorim, E. M. Dunne, A. J. Downard, S. Ehrhart, A. Franchin, M.K. Kajos, J. Kirkby, A. Kürten, T. Nieminen, V. Makhmutov, S. Mathot, P. Miettinen, A. Onnela, T. Petäjä, A. Praplan, F. D. Santos, S. Schallhart, M. Sipilä, Y. Stozhkov, A. Tomé, P. Vaattovaara, D. Wimmer, A. Prevot, J. Dommen, N. M. Donahue, R.C. Flagan, E. Weingartner, Y. Viisanen, I. Riipinen, A. Hansel, J. Curtius, M. Kulmala, D. R. Worsnop, U. Baltensperger, H. Wex, F. Stratmann, and A. Laaksonen
Atmos. Chem. Phys., 13, 5587–5600, https://doi.org/10.5194/acp-13-5587-2013, https://doi.org/10.5194/acp-13-5587-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Stratosphere | Science Focus: Physics (physical properties and processes)
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Particle number concentrations and size distributions in the stratosphere: implications of nucleation mechanisms and particle microphysics
Interactive stratospheric aerosol models' response to different amounts and altitudes of SO2 injection during the 1991 Pinatubo eruption
Climate response to off-equatorial stratospheric sulfur injections in three Earth system models – Part 2: Stratospheric and free-tropospheric response
The effect of ash, water vapor, and heterogeneous chemistry on the evolution of a Pinatubo-size volcanic cloud
Dynamical perturbation of the stratosphere by a pyrocumulonimbus injection of carbonaceous aerosols
Important role of stratospheric injection height for the distribution and radiative forcing of smoke aerosol from the 2019–2020 Australian wildfires
Volcanic stratospheric injections up to 160 Tg(S) yield a Eurasian winter warming indistinguishable from internal variability
Assessing the consequences of including aerosol absorption in potential stratospheric aerosol injection climate intervention strategies
An approach to sulfate geoengineering with surface emissions of carbonyl sulfide
Online treatment of eruption dynamics improves the volcanic ash and SO2 dispersion forecast: case of the 2019 Raikoke eruption
The impact of stratospheric aerosol intervention on the North Atlantic and Quasi-Biennial Oscillations in the Geoengineering Model Intercomparison Project (GeoMIP) G6sulfur experiment
An interactive stratospheric aerosol model intercomparison of solar geoengineering by stratospheric injection of SO2 or accumulation-mode sulfuric acid aerosols
Limitations of assuming internal mixing between different aerosol species: a case study with sulfate geoengineering simulations
Dependency of the impacts of geoengineering on the stratospheric sulfur injection strategy – Part 1: Intercomparison of modal and sectional aerosol modules
The long-term transport and radiative impacts of the 2017 British Columbia pyrocumulonimbus smoke aerosols in the stratosphere
Identifying the sources of uncertainty in climate model simulations of solar radiation modification with the G6sulfur and G6solar Geoengineering Model Intercomparison Project (GeoMIP) simulations
Harnessing stratospheric diffusion barriers for enhanced climate geoengineering
Comparing different generations of idealized solar geoengineering simulations in the Geoengineering Model Intercomparison Project (GeoMIP)
Model physics and chemistry causing intermodel disagreement within the VolMIP-Tambora Interactive Stratospheric Aerosol ensemble
North Atlantic Oscillation response in GeoMIP experiments G6solar and G6sulfur: why detailed modelling is needed for understanding regional implications of solar radiation management
Scant evidence for a volcanically forced winter warming over Eurasia following the Krakatau eruption of August 1883
Differing responses of the quasi-biennial oscillation to artificial SO2 injections in two global models
Revisiting the Agung 1963 volcanic forcing – impact of one or two eruptions
Northern Hemisphere continental winter warming following the 1991 Mt. Pinatubo eruption: reconciling models and observations
Upper tropospheric ice sensitivity to sulfate geoengineering
Stratospheric aerosol radiative forcing simulated by the chemistry climate model EMAC using Aerosol CCI satellite data
Dynamical response of Mediterranean precipitation to greenhouse gases and aerosols
Global radiative effects of solid fuel cookstove aerosol emissions
Model simulations of the chemical and aerosol microphysical evolution of the Sarychev Peak 2009 eruption cloud compared to in situ and satellite observations
Sensitivity of the radiative forcing by stratospheric sulfur geoengineering to the amount and strategy of the SO2injection studied with the LMDZ-S3A model
Sulfur deposition changes under sulfate geoengineering conditions: quasi-biennial oscillation effects on the transport and lifetime of stratospheric aerosols
Changing transport processes in the stratosphere by radiative heating of sulfate aerosols
Equatorward dispersion of a high-latitude volcanic plume and its relation to the Asian summer monsoon: a case study of the Sarychev eruption in 2009
Sulfate geoengineering impact on methane transport and lifetime: results from the Geoengineering Model Intercomparison Project (GeoMIP)
Radiative and climate effects of stratospheric sulfur geoengineering using seasonally varying injection areas
Volcanic ash modeling with the online NMMB-MONARCH-ASH v1.0 model: model description, case simulation, and evaluation
Sulfate geoengineering: a review of the factors controlling the needed injection of sulfur dioxide
Climatic impacts of stratospheric geoengineering with sulfate, black carbon and titania injection
Radiative and climate impacts of a large volcanic eruption during stratospheric sulfur geoengineering
Climate extremes in multi-model simulations of stratospheric aerosol and marine cloud brightening climate engineering
What is the limit of climate engineering by stratospheric injection of SO2?
Quasi-biennial oscillation of the tropical stratospheric aerosol layer
The impact of volcanic aerosol on the Northern Hemisphere stratospheric polar vortex: mechanisms and sensitivity to forcing structure
Modeling the stratospheric warming following the Mt. Pinatubo eruption: uncertainties in aerosol extinctions
Christian von Savigny, Anna Lange, Christoph G. Hoffmann, and Alexei Rozanov
Atmos. Chem. Phys., 24, 2415–2422, https://doi.org/10.5194/acp-24-2415-2024, https://doi.org/10.5194/acp-24-2415-2024, 2024
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It is well known that volcanic eruptions strongly affect the colours of the twilight sky. Typically, volcanic eruptions lead to enhanced reddish and violet twilight colours. In rare cases, however, volcanic eruptions can also lead to green sunsets. This study provides an explanation for the occurrence of these unusual green sunsets based on simulations with a radiative transfer model. Green volcanic sunsets require a sufficient stratospheric aerosol optical depth and specific aerosol sizes.
Jan Clemens, Bärbel Vogel, Lars Hoffmann, Sabine Griessbach, Nicole Thomas, Suvarna Fadnavis, Rolf Müller, Thomas Peter, and Felix Ploeger
Atmos. Chem. Phys., 24, 763–787, https://doi.org/10.5194/acp-24-763-2024, https://doi.org/10.5194/acp-24-763-2024, 2024
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The source regions of the Asian tropopause aerosol layer (ATAL) are debated. We use balloon-borne measurements of the layer above Nainital (India) in August 2016 and atmospheric transport models to find ATAL source regions. Most air originated from the Tibetan plateau. However, the measured ATAL was stronger when more air originated from the Indo-Gangetic Plain and weaker when more air originated from the Pacific. Hence, the results indicate important anthropogenic contributions to the ATAL.
Seyed Vahid Mousavi, Khalil Karami, Simone Tilmes, Helene Muri, Lili Xia, and Abolfazl Rezaei
Atmos. Chem. Phys., 23, 10677–10695, https://doi.org/10.5194/acp-23-10677-2023, https://doi.org/10.5194/acp-23-10677-2023, 2023
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Understanding atmospheric dust changes in the Middle East and North Africa (MENA) region under future climate scenarios is essential. By injecting sulfate aerosols into the stratosphere, stratospheric aerosol injection (SAI) geoengineering reflects some of the incoming sunlight back to space. This study shows that the MENA region would experience lower dust concentration under both SAI and RCP8.5 scenarios compared to the current climate (CTL) by the end of the century.
Fabian Senf, Bernd Heinold, Anne Kubin, Jason Müller, Roland Schrödner, and Ina Tegen
Atmos. Chem. Phys., 23, 8939–8958, https://doi.org/10.5194/acp-23-8939-2023, https://doi.org/10.5194/acp-23-8939-2023, 2023
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Wildfire smoke is a significant source of airborne atmospheric particles that can absorb sunlight. Extreme fires in particular, such as those during the 2019–2020 Australian wildfire season (Black Summer fires), can considerably affect our climate system. In the present study, we investigate the various effects of Australian smoke using a global climate model to clarify how the Earth's atmosphere, including its circulation systems, adjusted to the extraordinary amount of Australian smoke.
Alan Robock, Lili Xia, Cheryl S. Harrison, Joshua Coupe, Owen B. Toon, and Charles G. Bardeen
Atmos. Chem. Phys., 23, 6691–6701, https://doi.org/10.5194/acp-23-6691-2023, https://doi.org/10.5194/acp-23-6691-2023, 2023
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A nuclear war could produce a nuclear winter, with catastrophic consequences for global food supplies. Nuclear winter theory helped to end the nuclear arms race in the 1980s, but more than 10 000 nuclear weapons still exist. This means they can be used, by unstable leaders, accidently from technical malfunctions or human error, or by terrorists. Therefore, it is urgent for scientists to study these issues, broadly communicate their results, and work for the elimination of nuclear weapons.
Alice F. Wells, Andy Jones, Martin Osborne, Lilly Damany-Pearce, Daniel G. Partridge, and James M. Haywood
Atmos. Chem. Phys., 23, 3985–4007, https://doi.org/10.5194/acp-23-3985-2023, https://doi.org/10.5194/acp-23-3985-2023, 2023
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In 2019 the Raikoke volcano erupted explosively, emitting the largest injection of SO2 into the stratosphere since 2011. Observations indicated that a large amount of volcanic ash was also injected. Previous studies have identified that volcanic ash can prolong the lifetime of stratospheric aerosol optical depth, which we explore in UKESM1. Comparisons to observations suggest that including ash in model emission schemes can improve the representation of volcanic plumes in global climate models.
Fangqun Yu, Gan Luo, Arshad Arjunan Nair, Sebastian Eastham, Christina J. Williamson, Agnieszka Kupc, and Charles A. Brock
Atmos. Chem. Phys., 23, 1863–1877, https://doi.org/10.5194/acp-23-1863-2023, https://doi.org/10.5194/acp-23-1863-2023, 2023
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Particle number concentrations and size distributions in the stratosphere are studied through model simulations and comparisons with measurements. The nucleation scheme used in most of the solar geoengineering modeling studies overpredicts the nucleation rates and particle number concentrations in the stratosphere. The model based on updated nucleation schemes captures reasonably well some aspects of particle size distributions but misses some features. The possible reasons are discussed.
Ilaria Quaglia, Claudia Timmreck, Ulrike Niemeier, Daniele Visioni, Giovanni Pitari, Christina Brodowsky, Christoph Brühl, Sandip S. Dhomse, Henning Franke, Anton Laakso, Graham W. Mann, Eugene Rozanov, and Timofei Sukhodolov
Atmos. Chem. Phys., 23, 921–948, https://doi.org/10.5194/acp-23-921-2023, https://doi.org/10.5194/acp-23-921-2023, 2023
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The last very large explosive volcanic eruption we have measurements for is the eruption of Mt. Pinatubo in 1991. It is therefore often used as a benchmark for climate models' ability to reproduce these kinds of events. Here, we compare available measurements with the results from multiple experiments conducted with climate models interactively simulating the aerosol cloud formation.
Ewa M. Bednarz, Daniele Visioni, Ben Kravitz, Andy Jones, James M. Haywood, Jadwiga Richter, Douglas G. MacMartin, and Peter Braesicke
Atmos. Chem. Phys., 23, 687–709, https://doi.org/10.5194/acp-23-687-2023, https://doi.org/10.5194/acp-23-687-2023, 2023
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Building on Part 1 of this two-part study, we demonstrate the role of biases in climatological circulation and specific aspects of model microphysics in driving the differences in simulated sulfate distributions amongst three Earth system models. We then characterize the simulated changes in stratospheric and free-tropospheric temperatures, ozone, water vapor, and large-scale circulation, elucidating the role of the above aspects in the surface responses discussed in Part 1.
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.
Giorgio Doglioni, Valentina Aquila, Sampa Das, Peter R. Colarco, and Dino Zardi
Atmos. Chem. Phys., 22, 11049–11064, https://doi.org/10.5194/acp-22-11049-2022, https://doi.org/10.5194/acp-22-11049-2022, 2022
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We use a global chemistry climate model to analyze the perturbations to the stratospheric dynamics caused by an injection of carbonaceous aerosol comparable to the one caused by a series of pyrocumulonimbi that formed over British Columbia, Canada on 13 August 2017. The injection of light-absorbing aerosol in an otherwise clean lower stratosphere causes the formation of long-lasting stratospheric anticyclones at the synoptic scale.
Bernd Heinold, Holger Baars, Boris Barja, Matthew Christensen, Anne Kubin, Kevin Ohneiser, Kerstin Schepanski, Nick Schutgens, Fabian Senf, Roland Schrödner, Diego Villanueva, and Ina Tegen
Atmos. Chem. Phys., 22, 9969–9985, https://doi.org/10.5194/acp-22-9969-2022, https://doi.org/10.5194/acp-22-9969-2022, 2022
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The extreme 2019–2020 Australian wildfires produced massive smoke plumes lofted into the lower stratosphere by pyrocumulonimbus convection. Most climate models do not adequately simulate the injection height of such intense fires. By combining aerosol-climate modeling with prescribed pyroconvective smoke injection and lidar observations, this study shows the importance of the representation of the most extreme wildfire events for estimating the atmospheric energy budget.
Kevin DallaSanta and Lorenzo M. Polvani
Atmos. Chem. Phys., 22, 8843–8862, https://doi.org/10.5194/acp-22-8843-2022, https://doi.org/10.5194/acp-22-8843-2022, 2022
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Volcanic eruptions cool the earth by reducing the amount of sunlight reaching the surface. Paradoxically, it has been suggested that they may also warm the surface, but the evidence for this is scant. Here, we show that a small warming can be seen in a climate model for large-enough eruptions. However, even for eruptions much larger than those that have occurred in the past two millennia, post-eruption winters over Eurasia are indistinguishable from those occurring without a prior eruption.
Jim M. Haywood, Andy Jones, Ben T. Johnson, and William McFarlane Smith
Atmos. Chem. Phys., 22, 6135–6150, https://doi.org/10.5194/acp-22-6135-2022, https://doi.org/10.5194/acp-22-6135-2022, 2022
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Simulations are presented investigating the influence of moderately absorbing aerosol in the stratosphere to combat the impacts of climate change. A number of detrimental impacts are noted compared to sulfate aerosol, including (i) reduced cooling efficiency, (ii) increased deficits in global precipitation, (iii) delays in the recovery of the stratospheric ozone hole, and (iv) disruption of the stratospheric circulation and the wintertime storm tracks that impact European precipitation.
Ilaria Quaglia, Daniele Visioni, Giovanni Pitari, and Ben Kravitz
Atmos. Chem. Phys., 22, 5757–5773, https://doi.org/10.5194/acp-22-5757-2022, https://doi.org/10.5194/acp-22-5757-2022, 2022
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Carbonyl sulfide is a gas that mixes very well in the atmosphere and can reach the stratosphere, where it reacts with sunlight and produces aerosol. Here we propose that, by increasing surface fluxes by an order of magnitude, the number of stratospheric aerosols produced may be enough to partially offset the warming produced by greenhouse gases. We explore what effect this would have on the atmospheric composition.
Julia Bruckert, Gholam Ali Hoshyaripour, Ákos Horváth, Lukas O. Muser, Fred J. Prata, Corinna Hoose, and Bernhard Vogel
Atmos. Chem. Phys., 22, 3535–3552, https://doi.org/10.5194/acp-22-3535-2022, https://doi.org/10.5194/acp-22-3535-2022, 2022
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Volcanic emissions endanger aviation and public health and also influence weather and climate. Forecasting the volcanic-plume dispersion is therefore a critical yet sophisticated task. Here, we show that explicit treatment of volcanic-plume dynamics and eruption source parameters significantly improves volcanic-plume dispersion forecasts. We further demonstrate the lofting of the SO2 due to a heating of volcanic particles by sunlight with major implications for volcanic aerosol research.
Andy Jones, Jim M. Haywood, Adam A. Scaife, Olivier Boucher, Matthew Henry, Ben Kravitz, Thibaut Lurton, Pierre Nabat, Ulrike Niemeier, Roland Séférian, Simone Tilmes, and Daniele Visioni
Atmos. Chem. Phys., 22, 2999–3016, https://doi.org/10.5194/acp-22-2999-2022, https://doi.org/10.5194/acp-22-2999-2022, 2022
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Simulations by six Earth-system models of geoengineering by introducing sulfuric acid aerosols into the tropical stratosphere are compared. A robust impact on the northern wintertime North Atlantic Oscillation is found, exacerbating precipitation reduction over parts of southern Europe. In contrast, the models show no consistency with regard to impacts on the Quasi-Biennial Oscillation, although results do indicate a risk that the oscillation could become locked into a permanent westerly phase.
Debra K. Weisenstein, Daniele Visioni, Henning Franke, Ulrike Niemeier, Sandro Vattioni, Gabriel Chiodo, Thomas Peter, and David W. Keith
Atmos. Chem. Phys., 22, 2955–2973, https://doi.org/10.5194/acp-22-2955-2022, https://doi.org/10.5194/acp-22-2955-2022, 2022
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This paper explores a potential method of geoengineering that could be used to slow the rate of change of climate over decadal scales. We use three climate models to explore how injections of accumulation-mode sulfuric acid aerosol change the large-scale stratospheric particle size distribution and radiative forcing response for the chosen scenarios. Radiative forcing per unit sulfur injected and relative to the change in aerosol burden is larger with particulate than with SO2 injections.
Daniele Visioni, Simone Tilmes, Charles Bardeen, Michael Mills, Douglas G. MacMartin, Ben Kravitz, and Jadwiga H. Richter
Atmos. Chem. Phys., 22, 1739–1756, https://doi.org/10.5194/acp-22-1739-2022, https://doi.org/10.5194/acp-22-1739-2022, 2022
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Aerosols are simulated in a simplified way in climate models: in the model analyzed here, they are represented in every grid as described by three simple logarithmic distributions, mixing all different species together. The size can evolve when new particles are formed, particles merge together to create a larger one or particles are deposited to the surface. This approximation normally works fairly well. Here we show however that when large amounts of sulfate are simulated, there are problems.
Anton Laakso, Ulrike Niemeier, Daniele Visioni, Simone Tilmes, and Harri Kokkola
Atmos. Chem. Phys., 22, 93–118, https://doi.org/10.5194/acp-22-93-2022, https://doi.org/10.5194/acp-22-93-2022, 2022
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The use of different spatio-temporal sulfur injection strategies with different magnitudes to create an artificial reflective aerosol layer to cool the climate is studied using sectional and modal aerosol schemes in a climate model. There are significant differences in the results depending on the aerosol microphysical module used. Different spatio-temporal injection strategies have a significant impact on the magnitude and zonal distribution of radiative forcing and atmospheric dynamics.
Sampa Das, Peter R. Colarco, Luke D. Oman, Ghassan Taha, and Omar Torres
Atmos. Chem. Phys., 21, 12069–12090, https://doi.org/10.5194/acp-21-12069-2021, https://doi.org/10.5194/acp-21-12069-2021, 2021
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Interactions of extreme fires with weather systems can produce towering smoke plumes that inject aerosols at very high altitudes (> 10 km). Three such major injections, largest at the time in terms of emitted aerosol mass, took place over British Columbia, Canada, in August 2017. We model the transport and impacts of injected aerosols on the radiation balance of the atmosphere. Our model results match the satellite-observed plume transport and residence time at these high altitudes very closely.
Daniele Visioni, Douglas G. MacMartin, Ben Kravitz, Olivier Boucher, Andy Jones, Thibaut Lurton, Michou Martine, Michael J. Mills, Pierre Nabat, Ulrike Niemeier, Roland Séférian, and Simone Tilmes
Atmos. Chem. Phys., 21, 10039–10063, https://doi.org/10.5194/acp-21-10039-2021, https://doi.org/10.5194/acp-21-10039-2021, 2021
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A new set of simulations is used to investigate commonalities, differences and sources of uncertainty when simulating the injection of SO2 in the stratosphere in order to mitigate the effects of climate change (solar geoengineering). The models differ in how they simulate the aerosols and how they spread around the stratosphere, resulting in differences in projected regional impacts. Overall, however, the models agree that aerosols have the potential to mitigate the warming produced by GHGs.
Nikolas O. Aksamit, Ben Kravitz, Douglas G. MacMartin, and George Haller
Atmos. Chem. Phys., 21, 8845–8861, https://doi.org/10.5194/acp-21-8845-2021, https://doi.org/10.5194/acp-21-8845-2021, 2021
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There exist robust and influential material features evolving within turbulent fluids that behave as the skeleton for fluid transport pathways. Recent developments in applied mathematics have made the identification of these time-varying structures more rigorous and insightful than ever. Using short-range wind forecasts, we detail how and why these material features can be exploited in an effort to optimize the spread of aerosols in the stratosphere for climate geoengineering.
Ben Kravitz, Douglas G. MacMartin, Daniele Visioni, Olivier Boucher, Jason N. S. Cole, Jim Haywood, Andy Jones, Thibaut Lurton, Pierre Nabat, Ulrike Niemeier, Alan Robock, Roland Séférian, and Simone Tilmes
Atmos. Chem. Phys., 21, 4231–4247, https://doi.org/10.5194/acp-21-4231-2021, https://doi.org/10.5194/acp-21-4231-2021, 2021
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This study investigates multi-model response to idealized geoengineering (high CO2 with solar reduction) across two different generations of climate models. We find that, with the exception of a few cases, the results are unchanged between the different generations. This gives us confidence that broad conclusions about the response to idealized geoengineering are robust.
Margot Clyne, Jean-Francois Lamarque, Michael J. Mills, Myriam Khodri, William Ball, Slimane Bekki, Sandip S. Dhomse, Nicolas Lebas, Graham Mann, Lauren Marshall, Ulrike Niemeier, Virginie Poulain, Alan Robock, Eugene Rozanov, Anja Schmidt, Andrea Stenke, Timofei Sukhodolov, Claudia Timmreck, Matthew Toohey, Fiona Tummon, Davide Zanchettin, Yunqian Zhu, and Owen B. Toon
Atmos. Chem. Phys., 21, 3317–3343, https://doi.org/10.5194/acp-21-3317-2021, https://doi.org/10.5194/acp-21-3317-2021, 2021
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This study finds how and why five state-of-the-art global climate models with interactive stratospheric aerosols differ when simulating the aftermath of large volcanic injections as part of the Model Intercomparison Project on the climatic response to Volcanic forcing (VolMIP). We identify and explain the consequences of significant disparities in the underlying physics and chemistry currently in some of the models, which are problems likely not unique to the models participating in this study.
Andy Jones, Jim M. Haywood, Anthony C. Jones, Simone Tilmes, Ben Kravitz, and Alan Robock
Atmos. Chem. Phys., 21, 1287–1304, https://doi.org/10.5194/acp-21-1287-2021, https://doi.org/10.5194/acp-21-1287-2021, 2021
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Two different methods of simulating a geoengineering scenario are compared using data from two different Earth system models. One method is very idealised while the other includes details of a plausible mechanism. The results from both models agree that the idealised approach does not capture an impact found when detailed modelling is included, namely that geoengineering induces a positive phase of the North Atlantic Oscillation which leads to warmer, wetter winters in northern Europe.
Lorenzo M. Polvani and Suzana J. Camargo
Atmos. Chem. Phys., 20, 13687–13700, https://doi.org/10.5194/acp-20-13687-2020, https://doi.org/10.5194/acp-20-13687-2020, 2020
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On the basis of questionable early studies, it is widely believed that low-latitude volcanic eruptions cause winter warming over Eurasia. However, we here demonstrate that the winter warming over Eurasia following the 1883 Krakatau eruption was unremarkable and, in all likelihood, unrelated to that eruption. Confirming similar findings for the 1991 Pinatubo eruption, the new research demonstrates that no detectable Eurasian winter warming is to be expected after eruptions of similar magnitude.
Ulrike Niemeier, Jadwiga H. Richter, and Simone Tilmes
Atmos. Chem. Phys., 20, 8975–8987, https://doi.org/10.5194/acp-20-8975-2020, https://doi.org/10.5194/acp-20-8975-2020, 2020
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Artificial injections of SO2 into the tropical stratosphere show an impact on the quasi-biennial oscillation (QBO). Different numerical models show only qualitatively but not quantitatively consistent impacts. We show for two models that the response of the QBO is similar when a similar stratospheric heating rate is induced by SO2 injections of different amounts. The reason is very different vertical advection in the two models resulting in different aerosol burden and heating of the aerosols.
Ulrike Niemeier, Claudia Timmreck, and Kirstin Krüger
Atmos. Chem. Phys., 19, 10379–10390, https://doi.org/10.5194/acp-19-10379-2019, https://doi.org/10.5194/acp-19-10379-2019, 2019
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In 1963 Mt. Agung, Indonesia, showed unrest for several months. During this period,
two medium-sized eruptions injected SO2 into the stratosphere. Recent volcanic emission datasets include only one large eruption phase. Therefore, we compared model experiments, with (a) one larger eruption and (b) two eruptions as observed. The evolution of the volcanic cloud differs significantly between the two experiments. Both climatic eruptions should be taken into account.
Lorenzo M. Polvani, Antara Banerjee, and Anja Schmidt
Atmos. Chem. Phys., 19, 6351–6366, https://doi.org/10.5194/acp-19-6351-2019, https://doi.org/10.5194/acp-19-6351-2019, 2019
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This study provides compelling new evidence that the surface winter warming observed over the Northern Hemisphere continents following the 1991 eruption of Mt. Pinatubo was, very likely, completely unrelated to the eruption. This result has implications for earlier eruptions, as the evidence presented here demonstrates that the surface signal of even the very largest known eruptions may be swamped by the internal variability at high latitudes.
Daniele Visioni, Giovanni Pitari, Glauco di Genova, Simone Tilmes, and Irene Cionni
Atmos. Chem. Phys., 18, 14867–14887, https://doi.org/10.5194/acp-18-14867-2018, https://doi.org/10.5194/acp-18-14867-2018, 2018
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Many side effects of sulfate geoengineering have to be analyzed before the world can even consider deploying this method of solar radiation management. In particular, we show that ice clouds in the upper troposphere are modified by a sulfate injection, producing a change that (by allowing for more planetary radiation to escape to space) would produce a further cooling. This might be important when considering the necessary amount of sulfate that needs to be injected to achieve a certain target.
Christoph Brühl, Jennifer Schallock, Klaus Klingmüller, Charles Robert, Christine Bingen, Lieven Clarisse, Andreas Heckel, Peter North, and Landon Rieger
Atmos. Chem. Phys., 18, 12845–12857, https://doi.org/10.5194/acp-18-12845-2018, https://doi.org/10.5194/acp-18-12845-2018, 2018
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Use of multi-instrument satellite data is important to get consistent simulations of aerosol radiative forcing by a complex chemistry climate model, here with a main focus on the lower stratosphere. The satellite data at different wavelengths together with the patterns in the simulated size distribution point to a significant contribution from moist mineral dust lifted to the tropopause region by the Asian summer monsoon.
Tao Tang, Drew Shindell, Bjørn H. Samset, Oliviér Boucher, Piers M. Forster, Øivind Hodnebrog, Gunnar Myhre, Jana Sillmann, Apostolos Voulgarakis, Timothy Andrews, Gregory Faluvegi, Dagmar Fläschner, Trond Iversen, Matthew Kasoar, Viatcheslav Kharin, Alf Kirkevåg, Jean-Francois Lamarque, Dirk Olivié, Thomas Richardson, Camilla W. Stjern, and Toshihiko Takemura
Atmos. Chem. Phys., 18, 8439–8452, https://doi.org/10.5194/acp-18-8439-2018, https://doi.org/10.5194/acp-18-8439-2018, 2018
Yaoxian Huang, Nadine Unger, Trude Storelvmo, Kandice Harper, Yiqi Zheng, and Chris Heyes
Atmos. Chem. Phys., 18, 5219–5233, https://doi.org/10.5194/acp-18-5219-2018, https://doi.org/10.5194/acp-18-5219-2018, 2018
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We apply a global 3-D climate model to quantify the climate impacts of carbonaceous aerosols from solid fuel cookstove emissions. Without black carbon (BC) serving as ice nuclei (IN), global and Indian solid fuel cookstove aerosol emissions have net global cooling impacts. However, when BC acts as IN, the net sign of radiative impacts of carbonaceous aerosols from solid fuel cookstove emissions varies with the choice of maximum freezing efficiency of BC during ice cloud formation.
Thibaut Lurton, Fabrice Jégou, Gwenaël Berthet, Jean-Baptiste Renard, Lieven Clarisse, Anja Schmidt, Colette Brogniez, and Tjarda J. Roberts
Atmos. Chem. Phys., 18, 3223–3247, https://doi.org/10.5194/acp-18-3223-2018, https://doi.org/10.5194/acp-18-3223-2018, 2018
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We quantify the chemical and microphysical effects of volcanic SO2 and HCl from the June 2009 Sarychev Peak eruption using a comprehensive aerosol–chemistry model combined with in situ measurements and satellite retrievals. Our results suggest that previous studies underestimated the eruption's atmospheric and climatic impact, mainly because previous model-to-satellite comparisons had to make assumptions about the aerosol size distribution and were based on biased satellite retrievals of AOD.
Christoph Kleinschmitt, Olivier Boucher, and Ulrich Platt
Atmos. Chem. Phys., 18, 2769–2786, https://doi.org/10.5194/acp-18-2769-2018, https://doi.org/10.5194/acp-18-2769-2018, 2018
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We use a state-of-the-art stratospheric aerosol model to study geoengineering through stratospheric sulfur injections. We find that the efficiency may decrease more drastically for larger injections than previously estimated and that injections at higher altitude are not more effective. This study may provide additional evidence that this proposed geoengineering technique is still more complicated, probably less effective, and may implicate stronger side effects than initially thought.
Daniele Visioni, Giovanni Pitari, Paolo Tuccella, and Gabriele Curci
Atmos. Chem. Phys., 18, 2787–2808, https://doi.org/10.5194/acp-18-2787-2018, https://doi.org/10.5194/acp-18-2787-2018, 2018
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Sulfate geoengineering is a proposed technique that would mimic explosive volcanic eruptions by injecting sulfur dioxide (SO2) into the stratosphere to counteract global warming produced by greenhouse gases by reflecting part of the incoming solar radiation. In this study we use two models to simulate how the injected aerosols would react to dynamical changes in the stratosphere (due to the quasi-biennial oscillation - QBO) and how this would affect the deposition of sulfate at the surface.
Ulrike Niemeier and Hauke Schmidt
Atmos. Chem. Phys., 17, 14871–14886, https://doi.org/10.5194/acp-17-14871-2017, https://doi.org/10.5194/acp-17-14871-2017, 2017
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An artificial stratospheric sulfur layer heats the lower stratosphere which impacts stratospheric dynamics and transport. The quasi-biennial oscillation shuts down due to the heated sulfur layer which impacts the meridional transport of the sulfate aerosols. The tropical confinement of the sulfate is stronger and the radiative forcing efficiency of the aerosol layer decreases compared to previous studies, as does the forcing when increasing the injection height.
Xue Wu, Sabine Griessbach, and Lars Hoffmann
Atmos. Chem. Phys., 17, 13439–13455, https://doi.org/10.5194/acp-17-13439-2017, https://doi.org/10.5194/acp-17-13439-2017, 2017
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This study is focused on the Sarychev eruption in 2009. Based on Lagrangian model simulations and satellite data, the equatorward transport of the plume and aerosol from the Sarychev eruption is confirmed, and the transport is facilitated by the Asian summer monsoon anticyclonic circulations. The aerosol transported to the tropics remained for months and dispersed upward, which could make the Sarychev eruption have a similar global climate impact as a tropical volcanic eruption.
Daniele Visioni, Giovanni Pitari, Valentina Aquila, Simone Tilmes, Irene Cionni, Glauco Di Genova, and Eva Mancini
Atmos. Chem. Phys., 17, 11209–11226, https://doi.org/10.5194/acp-17-11209-2017, https://doi.org/10.5194/acp-17-11209-2017, 2017
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Sulfate geoengineering (SG), the sustained injection of SO2 in the lower stratosphere, is being discussed as a way to counterbalance surface warming, mimicking volcanic eruptions. In this paper, we analyse results from two models part of the GeoMIP project in order to understand the effect SG might have on the concentration and lifetime of methane, which acts in the atmosphere as a greenhouse gas. Understanding possible side effects of SG is a crucial step if its viability is to be assessed.
Anton Laakso, Hannele Korhonen, Sami Romakkaniemi, and Harri Kokkola
Atmos. Chem. Phys., 17, 6957–6974, https://doi.org/10.5194/acp-17-6957-2017, https://doi.org/10.5194/acp-17-6957-2017, 2017
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Based on simulations, equatorial stratospheric sulfur injections have shown to be an efficient strategy to counteract ongoing global warming. However, equatorial injections would result in relatively larger cooling in low latitudes than in high latitudes. This together with greenhouse-gas-induced warming would lead to cooling in the Equator and warming in the high latitudes. Results of this study show that a more optimal cooling effect is achieved by varying the injection area seasonally.
Alejandro Marti, Arnau Folch, Oriol Jorba, and Zavisa Janjic
Atmos. Chem. Phys., 17, 4005–4030, https://doi.org/10.5194/acp-17-4005-2017, https://doi.org/10.5194/acp-17-4005-2017, 2017
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We describe and evaluate NMMB-MONARCH-ASH, a novel online multi-scale meteorological and transport model developed at the BSC-CNS capable of forecasting the dispersal and deposition of volcanic ash. The forecast skills of the model have been validated and they improve on those from traditional operational offline (decoupled) models. The results support the use of online coupled models to aid civil aviation and emergency management during a crisis such as the 2010 eruption of Eyjafjallajökull.
Daniele Visioni, Giovanni Pitari, and Valentina Aquila
Atmos. Chem. Phys., 17, 3879–3889, https://doi.org/10.5194/acp-17-3879-2017, https://doi.org/10.5194/acp-17-3879-2017, 2017
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This review paper summarizes the state-of-the-art knowledge of the direct and indirect side effects of sulfate geoengineering, that is, the injection of sulfur dioxide into the stratosphere in order to offset the warming caused by the anthropic increase in greenhouse gasses. An overview of the various effects and their uncertainties, using results from published scientific articles, may help fine-tune the best amount of sulfate to be injected in an eventual realization of the experiment.
Anthony C. Jones, James M. Haywood, and Andy Jones
Atmos. Chem. Phys., 16, 2843–2862, https://doi.org/10.5194/acp-16-2843-2016, https://doi.org/10.5194/acp-16-2843-2016, 2016
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In this paper we assess the potential climatic impacts of geoengineering with sulfate, black carbon and titania injection strategies. We find that black carbon injection results in severe stratospheric warming and precipitation impacts, and therefore black carbon is unsuitable for geoengineering purposes. As the injection rates and climatic impacts for titania are close to those for sulfate, there appears little benefit of using titania when compared to injection of sulfur dioxide.
A. Laakso, H. Kokkola, A.-I. Partanen, U. Niemeier, C. Timmreck, K. E. J. Lehtinen, H. Hakkarainen, and H. Korhonen
Atmos. Chem. Phys., 16, 305–323, https://doi.org/10.5194/acp-16-305-2016, https://doi.org/10.5194/acp-16-305-2016, 2016
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We have studied the impacts of a volcanic eruption during solar radiation management (SRM) using an aerosol-climate model ECHAM5-HAM-SALSA and an Earth system model MPI-ESM. A volcanic eruption during stratospheric sulfur geoengineering would lead to larger particles and smaller amount of new particles than if an volcano erupts in normal atmospheric conditions. Thus, volcanic eruption during SRM would lead to only a small additional cooling which would last for a significantly shorter period.
V. N. Aswathy, O. Boucher, M. Quaas, U. Niemeier, H. Muri, J. Mülmenstädt, and J. Quaas
Atmos. Chem. Phys., 15, 9593–9610, https://doi.org/10.5194/acp-15-9593-2015, https://doi.org/10.5194/acp-15-9593-2015, 2015
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Simulations conducted in the GeoMIP and IMPLICC model intercomparison studies for climate engineering by stratospheric sulfate injection and marine cloud brightening via sea salt are analysed and compared to the reference scenario RCP4.5. The focus is on extremes in surface temperature and precipitation. It is found that the extreme changes mostly follow the mean changes and that extremes are also in general well mitigated, except for in polar regions.
U. Niemeier and C. Timmreck
Atmos. Chem. Phys., 15, 9129–9141, https://doi.org/10.5194/acp-15-9129-2015, https://doi.org/10.5194/acp-15-9129-2015, 2015
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The injection of sulfur dioxide is considered as an option for solar radiation management. We have calculated the effects of SO2 injections up to 100 Tg(S)/y. Our calculations show that the forcing efficiency of the injection decays exponentially. This result implies that SO2 injections in the order of 6 times Mt. Pinatubo eruptions per year are required to keep temperatures constant at that anticipated for 2020, whilst maintaining business as usual emission conditions.
R. Hommel, C. Timmreck, M. A. Giorgetta, and H. F. Graf
Atmos. Chem. Phys., 15, 5557–5584, https://doi.org/10.5194/acp-15-5557-2015, https://doi.org/10.5194/acp-15-5557-2015, 2015
M. Toohey, K. Krüger, M. Bittner, C. Timmreck, and H. Schmidt
Atmos. Chem. Phys., 14, 13063–13079, https://doi.org/10.5194/acp-14-13063-2014, https://doi.org/10.5194/acp-14-13063-2014, 2014
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Earth system model simulations are used to investigate the impact of volcanic aerosol forcing on stratospheric dynamics, e.g. the Northern Hemisphere (NH) polar vortex. We find that mechanisms linking aerosol heating and high-latitude dynamics are not as direct as often assumed; high-latitude effects result from changes in stratospheric circulation and related vertical motions. The simulated responses also show evidence of being sensitive to the structure of the volcanic forcing used.
F. Arfeuille, B. P. Luo, P. Heckendorn, D. Weisenstein, J. X. Sheng, E. Rozanov, M. Schraner, S. Brönnimann, L. W. Thomason, and T. Peter
Atmos. Chem. Phys., 13, 11221–11234, https://doi.org/10.5194/acp-13-11221-2013, https://doi.org/10.5194/acp-13-11221-2013, 2013
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Short summary
Recent research has analyzed the formation of a particle (CN) layer in the stratosphere above Antarctica after sunrise. We investigate the CN layer formation processes with our particle formation model and derive sulfuric acid profiles (no measurements exist). Our study confirms existing explanations and gives more insights into the formation process, leading to higher derived concentrations. Therefore, this paper improves our understanding of the processes in the high atmosphere.
Recent research has analyzed the formation of a particle (CN) layer in the stratosphere above...
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