Articles | Volume 21, issue 5
https://doi.org/10.5194/acp-21-3827-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-21-3827-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Technical note
| 
15 Mar 2021
Technical note |
| 15 Mar 2021
| 15 Mar 2021
Technical note: The enhancement limit of coagulation scavenging of small charged particles
Naser G. A. Mahfouz
Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA, USA
Department of Chemical Engineering, Carnegie Mellon University, Pittsburgh, PA, USA
Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA, USA
Department of Chemical Engineering, Carnegie Mellon University, Pittsburgh, PA, USA
Department of Chemistry, Carnegie Mellon University, Pittsburgh, PA, USA
Department of Engineering and Public Policy, Carnegie Mellon University, Pittsburgh, PA, USA
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Yuanyuan Luo, Lauri Franzon, Jiangyi Zhang, Nina Sarnela, Neil M. Donahue, Theo Kurtén, and Mikael Ehn
EGUsphere, https://doi.org/10.5194/egusphere-2024-3323, https://doi.org/10.5194/egusphere-2024-3323, 2024
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This study explores the formation of accretion products from reactions involving highly reactive compounds, Criegee intermediates. We focused on three types of terpenes, common in nature, and their reactions with specific acids. Our findings reveal that these reactions efficiently produce expected compounds. This research enhances our understanding of how these reactions affect air quality and climate by contributing to aerosol formation, crucial for atmospheric chemistry.
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.
Chao Yan, Yicheng Shen, Dominik Stolzenburg, Lubna Dada, Ximeng Qi, Simo Hakala, Anu-Maija Sundström, Yishuo Guo, Antti Lipponen, Tom V. Kokkonen, Jenni Kontkanen, Runlong Cai, Jing Cai, Tommy Chan, Liangduo Chen, Biwu Chu, Chenjuan Deng, Wei Du, Xiaolong Fan, Xu-Cheng He, Juha Kangasluoma, Joni Kujansuu, Mona Kurppa, Chang Li, Yiran Li, Zhuohui Lin, Yiliang Liu, Yuliang Liu, Yiqun Lu, Wei Nie, Jouni Pulliainen, Xiaohui Qiao, Yonghong Wang, Yifan Wen, Ye Wu, Gan Yang, Lei Yao, Rujing Yin, Gen Zhang, Shaojun Zhang, Feixue Zheng, Ying Zhou, Antti Arola, Johanna Tamminen, Pauli Paasonen, Yele Sun, Lin Wang, Neil M. Donahue, Yongchun Liu, Federico Bianchi, Kaspar R. Daellenbach, Douglas R. Worsnop, Veli-Matti Kerminen, Tuukka Petäjä, Aijun Ding, Jingkun Jiang, and Markku Kulmala
Atmos. Chem. Phys., 22, 12207–12220, https://doi.org/10.5194/acp-22-12207-2022, https://doi.org/10.5194/acp-22-12207-2022, 2022
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Atmospheric new particle formation (NPF) is a dominant source of atmospheric ultrafine particles. In urban environments, traffic emissions are a major source of primary pollutants, but their contribution to NPF remains under debate. During the COVID-19 lockdown, traffic emissions were significantly reduced, providing a unique chance to examine their relevance to NPF. Based on our comprehensive measurements, we demonstrate that traffic emissions alone are not able to explain the NPF in Beijing.
Dalrin Ampritta Amaladhasan, Claudia Heyn, Christopher R. Hoyle, Imad El Haddad, Miriam Elser, Simone M. Pieber, Jay G. Slowik, Antonio Amorim, Jonathan Duplissy, Sebastian Ehrhart, Vladimir Makhmutov, Ugo Molteni, Matti Rissanen, Yuri Stozhkov, Robert Wagner, Armin Hansel, Jasper Kirkby, Neil M. Donahue, Rainer Volkamer, Urs Baltensperger, Martin Gysel-Beer, and Andreas Zuend
Atmos. Chem. Phys., 22, 215–244, https://doi.org/10.5194/acp-22-215-2022, https://doi.org/10.5194/acp-22-215-2022, 2022
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We use a combination of models for gas-phase chemical reactions and equilibrium gas–particle partitioning of isoprene-derived secondary organic aerosols (SOAs) informed by dark ozonolysis experiments conducted in the CLOUD chamber. Our predictions cover high to low relative humidities (RHs) and quantify how SOA mass yields are enhanced at high RH as well as the impact of inorganic seeds of distinct hygroscopicities and acidities on the coupled partitioning of water and semi-volatile organics.
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.
Yuliang Liu, Wei Nie, Yuanyuan Li, Dafeng Ge, Chong Liu, Zhengning Xu, Liangduo Chen, Tianyi Wang, Lei Wang, Peng Sun, Ximeng Qi, Jiaping Wang, Zheng Xu, Jian Yuan, Chao Yan, Yanjun Zhang, Dandan Huang, Zhe Wang, Neil M. Donahue, Douglas Worsnop, Xuguang Chi, Mikael Ehn, and Aijun Ding
Atmos. Chem. Phys., 21, 14789–14814, https://doi.org/10.5194/acp-21-14789-2021, https://doi.org/10.5194/acp-21-14789-2021, 2021
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Oxygenated organic molecules (OOMs) are crucial intermediates linking volatile organic compounds to secondary organic aerosols. Using nitrate time-of-flight chemical ionization mass spectrometry in eastern China, we performed positive matrix factorization (PMF) on binned OOM mass spectra. We reconstructed over 1000 molecules from 14 derived PMF factors and identified about 72 % of the observed OOMs as organic nitrates, highlighting the decisive role of NOx in OOM formation in populated areas.
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.
Chuan Ping Lee, Mihnea Surdu, David M. Bell, Houssni Lamkaddam, Mingyi Wang, Farnoush Ataei, Victoria Hofbauer, Brandon Lopez, Neil M. Donahue, Josef Dommen, Andre S. H. Prevot, Jay G. Slowik, Dongyu Wang, Urs Baltensperger, and Imad El Haddad
Atmos. Meas. Tech., 14, 5913–5923, https://doi.org/10.5194/amt-14-5913-2021, https://doi.org/10.5194/amt-14-5913-2021, 2021
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Extractive electrospray ionization mass spectrometry (EESI-MS) has been deployed for high throughput online detection of particles with minimal fragmentation. Our study elucidates the extraction mechanism between the particles and electrospray (ES) droplets of different properties. The results show that the extraction rate is likely affected by the coagulation rate between the particles and ES droplets. Once coagulated, the particles undergo complete extraction within the ES droplet.
Wei Huang, Haiyan Li, Nina Sarnela, Liine Heikkinen, Yee Jun Tham, Jyri Mikkilä, Steven J. Thomas, Neil M. Donahue, Markku Kulmala, and Federico Bianchi
Atmos. Chem. Phys., 21, 8961–8977, https://doi.org/10.5194/acp-21-8961-2021, https://doi.org/10.5194/acp-21-8961-2021, 2021
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We show full characterization of gaseous organic compounds in a boreal forest. Molecular composition and volatility of gaseous organic compounds with different oxidation extents (from volatile organic compounds to highly oxygenated organic molecules) were investigated and discussed. We provide a more comprehensive understanding of atmospheric organic compounds in this boreal forest and new insights into interpreting ambient measurements or testing and improving parameterizations in models.
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.
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.
Meredith Schervish and Neil M. Donahue
Atmos. Chem. Phys., 20, 1183–1199, https://doi.org/10.5194/acp-20-1183-2020, https://doi.org/10.5194/acp-20-1183-2020, 2020
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Gas-phase autoxidation of organics can generate highly oxygenated organic molecules (HOMs) and thus increase secondary organic aerosol production and enable new-particle formation. Here we explicitly represent the generation of HOMs via peroxy radical chemistry and resolve the products based on volatility and O : C. Using experimentally constrained assumptions about autoxidation and dimerization reactions, we see suppression of HOM formation under low-temperature and high-NOx conditions.
Ningxin Wang, Spiro D. Jorga, Jeffery R. Pierce, Neil M. Donahue, and Spyros N. Pandis
Atmos. Meas. Tech., 11, 6577–6588, https://doi.org/10.5194/amt-11-6577-2018, https://doi.org/10.5194/amt-11-6577-2018, 2018
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The interaction of particles with the chamber walls has been a significant source of uncertainty when analyzing results of secondary organic aerosol formation experiments performed in Teflon chambers. We evaluated the performance of several particle wall-loss correction methods for aging experiments of α-pinene ozonolysis products. Experimental procedures are proposed for the characterization of particle losses during different stages of these experiments.
Xiangyu Pei, Mattias Hallquist, Axel C. Eriksson, Joakim Pagels, Neil M. Donahue, Thomas Mentel, Birgitta Svenningsson, William Brune, and Ravi Kant Pathak
Atmos. Chem. Phys., 18, 9845–9860, https://doi.org/10.5194/acp-18-9845-2018, https://doi.org/10.5194/acp-18-9845-2018, 2018
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The findings in this study show that morphological transformation of soot occurs via two key complementary and sequential processes, i.e., void filling in the particle and its diameter growth. To quantify the state of morphological transformation, i.e., the utilization of material for filling and growth during the condensation processes, a framework was developed which can further be utilized to quantify the effect of condensed material on the optical and hygroscopic properties of soot.
Penglin Ye, Yunliang Zhao, Wayne K. Chuang, Allen L. Robinson, and Neil M. Donahue
Atmos. Chem. Phys., 18, 6171–6186, https://doi.org/10.5194/acp-18-6171-2018, https://doi.org/10.5194/acp-18-6171-2018, 2018
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This work describes experiments to constrain the production of secondary organic aerosol from pinanediol, a semi-volatile oxidation product of α-pinene. Our results and the implications for SOA aging are directly relevant to the atmospheric chemistry community because they connect new-particle formation experiments and SOA formation experiments. The oxidation conditions are typically different and experiments are also influenced in different ways by wall losses of condensible vapors.
Ningxin Wang, Evangelia Kostenidou, Neil M. Donahue, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 3589–3601, https://doi.org/10.5194/acp-18-3589-2018, https://doi.org/10.5194/acp-18-3589-2018, 2018
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This study investigates aging in the α-pinene ozonolysis system with hydroxyl radicals (OH) through smog chamber experiments. After an equivalent of 2–4 days of typical atmospheric oxidation conditions, homogeneous OH oxidation of the α-pinene ozonolysis products resulted in a 20–40 % net increase in the organic aerosol concentration and an increase in aerosol O : C by up to 0.04. The relative humidity in the 5–50 % range had a minimum effect on aging.
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
Wayne K. Chuang and Neil M. Donahue
Atmos. Chem. Phys., 17, 10019–10036, https://doi.org/10.5194/acp-17-10019-2017, https://doi.org/10.5194/acp-17-10019-2017, 2017
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Experiments on organic aerosol formation are important for our understanding of climate. Recent experiments on the reaction of ozone with alpha-pinene showed high production of extremely low-volatility organics. This appeared to contradict prior volatility distributions derived from equilibrium partitioning. We examined this using a dynamic volatility basis set model and found that the delay between the production and condensation of organics is integral to reconciling this difference.
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.
Ellis Shipley Robinson, Timothy B. Onasch, Douglas Worsnop, and Neil M. Donahue
Atmos. Meas. Tech., 10, 1139–1154, https://doi.org/10.5194/amt-10-1139-2017, https://doi.org/10.5194/amt-10-1139-2017, 2017
Nga Lee Ng, Steven S. Brown, Alexander T. Archibald, Elliot Atlas, Ronald C. Cohen, John N. Crowley, Douglas A. Day, Neil M. Donahue, Juliane L. Fry, Hendrik Fuchs, Robert J. Griffin, Marcelo I. Guzman, Hartmut Herrmann, Alma Hodzic, Yoshiteru Iinuma, José L. Jimenez, Astrid Kiendler-Scharr, Ben H. Lee, Deborah J. Luecken, Jingqiu Mao, Robert McLaren, Anke Mutzel, Hans D. Osthoff, Bin Ouyang, Benedicte Picquet-Varrault, Ulrich Platt, Havala O. T. Pye, Yinon Rudich, Rebecca H. Schwantes, Manabu Shiraiwa, Jochen Stutz, Joel A. Thornton, Andreas Tilgner, Brent J. Williams, and Rahul A. Zaveri
Atmos. Chem. Phys., 17, 2103–2162, https://doi.org/10.5194/acp-17-2103-2017, https://doi.org/10.5194/acp-17-2103-2017, 2017
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Oxidation of biogenic volatile organic compounds by NO3 is an important interaction between anthropogenic
and natural emissions. This review results from a June 2015 workshop and includes the recent literature
on kinetics, mechanisms, organic aerosol yields, and heterogeneous chemistry; advances in analytical
instrumentation; the current state NO3-BVOC chemistry in atmospheric models; and critical needs for
future research in modeling, field observations, and laboratory studies.
Adam T. Ahern, Ramachandran Subramanian, Georges Saliba, Eric M. Lipsky, Neil M. Donahue, and Ryan C. Sullivan
Atmos. Meas. Tech., 9, 6117–6137, https://doi.org/10.5194/amt-9-6117-2016, https://doi.org/10.5194/amt-9-6117-2016, 2016
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The SP-AMS exhibited a different sensitivity to black carbon vs. potassium as more SOA mass was condensed onto biomass burning particles. The SP-AMS's sensitivity to BC mass did not plateau following successive SOA coatings, despite achieving high OA : BC mass ratios > 9. A laser ablation single-particle mass spectrometer exhibited a positive correlation to the condensed SOA mass on individual soot particles, demonstrating its ability to obtain mass quantitative measurements from complex matrices.
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.
Emma Järvinen, Karoliina Ignatius, Leonid Nichman, Thomas B. Kristensen, Claudia Fuchs, Christopher R. Hoyle, Niko Höppel, Joel C. Corbin, Jill Craven, Jonathan Duplissy, Sebastian Ehrhart, Imad El Haddad, Carla Frege, Hamish Gordon, Tuija Jokinen, Peter Kallinger, Jasper Kirkby, Alexei Kiselev, Karl-Heinz Naumann, Tuukka Petäjä, Tamara Pinterich, Andre S. H. Prevot, Harald Saathoff, Thea Schiebel, Kamalika Sengupta, Mario Simon, Jay G. Slowik, Jasmin Tröstl, Annele Virtanen, Paul Vochezer, Steffen Vogt, Andrea C. Wagner, Robert Wagner, Christina Williamson, Paul M. Winkler, Chao Yan, Urs Baltensperger, Neil M. Donahue, Rick C. Flagan, Martin Gallagher, Armin Hansel, Markku Kulmala, Frank Stratmann, Douglas R. Worsnop, Ottmar Möhler, Thomas Leisner, and Martin Schnaiter
Atmos. Chem. Phys., 16, 4423–4438, https://doi.org/10.5194/acp-16-4423-2016, https://doi.org/10.5194/acp-16-4423-2016, 2016
Leonid Nichman, Claudia Fuchs, Emma Järvinen, Karoliina Ignatius, Niko Florian Höppel, Antonio Dias, Martin Heinritzi, Mario Simon, Jasmin Tröstl, Andrea Christine Wagner, Robert Wagner, Christina Williamson, Chao Yan, Paul James Connolly, James Robert Dorsey, Jonathan Duplissy, Sebastian Ehrhart, Carla Frege, Hamish Gordon, Christopher Robert Hoyle, Thomas Bjerring Kristensen, Gerhard Steiner, Neil McPherson Donahue, Richard Flagan, Martin William Gallagher, Jasper Kirkby, Ottmar Möhler, Harald Saathoff, Martin Schnaiter, Frank Stratmann, and António Tomé
Atmos. Chem. Phys., 16, 3651–3664, https://doi.org/10.5194/acp-16-3651-2016, https://doi.org/10.5194/acp-16-3651-2016, 2016
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Processes in the atmosphere are often governed by the physical and chemical properties of small cloud particles. Ice, water, and mixed clouds, as well as viscous aerosols, were formed under controlled conditions at the CLOUD-CERN facility. The experimental results show a link between cloud particle properties and their unique optical fingerprints. The classification map presented here allows easier discrimination between various particles such as viscous organic aerosol, salt, ice, and liquid.
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.
W. K. Chuang and N. M. Donahue
Atmos. Chem. Phys., 16, 123–134, https://doi.org/10.5194/acp-16-123-2016, https://doi.org/10.5194/acp-16-123-2016, 2016
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NOx is formed under high-temperature conditions such as combustion. When NOx enters the atmosphere, it alters the chemistry of organic emissions and can form organonitrates. Depending on the conditions, NOx may increase or decrease resulting aerosol concentrations. We expanded the two-dimensional volatility basis set (2D-VBS) to model organonitrates and the effect on aerosol concentrations. We discuss the mathematical framework of the model and include the code in the Supplement.
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.
L. Hildebrandt Ruiz, A. L. Paciga, K. M. Cerully, A. Nenes, N. M. Donahue, and S. N. Pandis
Atmos. Chem. Phys., 15, 8301–8313, https://doi.org/10.5194/acp-15-8301-2015, https://doi.org/10.5194/acp-15-8301-2015, 2015
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Secondary organic aerosol (SOA) is transformed after its initial formation. We explored the effects of this chemical aging on the composition, mass yield, volatility, and hygroscopicity of SOA formed from the photo-oxidation of small aromatic volatile organic compounds. Higher exposure to the hydroxyl radical resulted in different SOA composition, average carbon oxidation state, and mass yield. The vapor pressure of SOA formed under different conditions varied by as much as a factor of 30.
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. 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.
M. R. Canagaratna, J. L. Jimenez, J. H. Kroll, Q. Chen, S. H. Kessler, P. Massoli, L. Hildebrandt Ruiz, E. Fortner, L. R. Williams, K. R. Wilson, J. D. Surratt, N. M. Donahue, J. T. Jayne, and D. R. Worsnop
Atmos. Chem. Phys., 15, 253–272, https://doi.org/10.5194/acp-15-253-2015, https://doi.org/10.5194/acp-15-253-2015, 2015
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Atomic oxygen-to-carbon (O:C), hydrogen-to-carbon (H:C), and organic mass-to-organic carbon (OM:OC) ratios of ambient organic aerosol (OA) species provide key constraints for understanding their sources and impacts. Here an improved method for obtaining accurate O:C, H:C, and OM:OC with a widely used aerosol mass spectrometer is developed. These results imply that OA is more oxidized than previously estimated and indicate the need for new chemical mechanisms that simulate ambient oxidation.
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.
M. Sipilä, T. Jokinen, T. Berndt, S. Richters, R. Makkonen, N. M. Donahue, R. L. Mauldin III, T. Kurtén, P. Paasonen, N. Sarnela, M. Ehn, H. Junninen, M. P. Rissanen, J. Thornton, F. Stratmann, H. Herrmann, D. R. Worsnop, M. Kulmala, V.-M. Kerminen, and T. Petäjä
Atmos. Chem. Phys., 14, 12143–12153, https://doi.org/10.5194/acp-14-12143-2014, https://doi.org/10.5194/acp-14-12143-2014, 2014
B. N. Murphy, N. M. Donahue, A. L. Robinson, and S. N. Pandis
Atmos. Chem. Phys., 14, 5825–5839, https://doi.org/10.5194/acp-14-5825-2014, https://doi.org/10.5194/acp-14-5825-2014, 2014
S. H. Jathar, N. M. Donahue, P. J. Adams, and A. L. Robinson
Atmos. Chem. Phys., 14, 5771–5780, https://doi.org/10.5194/acp-14-5771-2014, https://doi.org/10.5194/acp-14-5771-2014, 2014
T. D. Gordon, A. A. Presto, A. A. May, N. T. Nguyen, E. M. Lipsky, N. M. Donahue, A. Gutierrez, M. Zhang, C. Maddox, P. Rieger, S. Chattopadhyay, H. Maldonado, M. M. Maricq, and A. L. Robinson
Atmos. Chem. Phys., 14, 4661–4678, https://doi.org/10.5194/acp-14-4661-2014, https://doi.org/10.5194/acp-14-4661-2014, 2014
E. R. Trump and N. M Donahue
Atmos. Chem. Phys., 14, 3691–3701, https://doi.org/10.5194/acp-14-3691-2014, https://doi.org/10.5194/acp-14-3691-2014, 2014
R. Saleh, C. J. Hennigan, G. R. McMeeking, W. K. Chuang, E. S. Robinson, H. Coe, N. M. Donahue, and A. L. Robinson
Atmos. Chem. Phys., 13, 7683–7693, https://doi.org/10.5194/acp-13-7683-2013, https://doi.org/10.5194/acp-13-7683-2013, 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: Troposphere | Science Focus: Physics (physical properties and processes)
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Impact of biomass burning aerosols (BBA) on the tropical African climate in an ocean–atmosphere–aerosol coupled climate model
Retrieval of refractive index and water content for the coating materials of aged black carbon aerosol based on optical properties: a theoretical analysis
Predicting hygroscopic growth of organosulfur aerosol particles using COSMOtherm
Dust aerosol from the Aralkum Desert influences the radiation budget and atmospheric dynamics of Central Asia
Global modeling of aerosol nucleation with a semi-explicit chemical mechanism for highly oxygenated organic molecules (HOMs)
Synergistic effects of the winter North Atlantic Oscillation (NAO) and El Niño–Southern Oscillation (ENSO) on dust activities in North China during the following spring
Aerosol composition, air quality, and boundary layer dynamics in the urban background of Stuttgart in winter
Measurement report: Source attribution and estimation of black carbon levels in an urban hotspot of the central Po Valley – an integrated approach combining high-resolution dispersion modelling and micro-aethalometers
Construction and Application of a Pollen Emissions Model based on Phenology and Random Forests
Microphysical modelling of aerosol scavenging by different types of clouds: description and validation of the approach
Insights into the sources of ultrafine particle numbers at six European urban sites obtained by investigating COVID-19 lockdowns
In-plume and out-of-plume analysis of aerosol–cloud interactions derived from the 2014–2015 Holuhraun volcanic eruption
Impacts of atmospheric circulation patterns and cloud inhibition on aerosol radiative effect and boundary layer structure during winter air pollution in Sichuan Basin, China
The effectiveness of solar radiation management for marine cloud brightening geoengineering by fine sea spray in worldwide different climatic regions
Accounting for Black Carbon Aging Process in a Two-way Coupled Meteorology – Air Quality Model
Investigating the sign of stratocumulus adjustments to aerosols in the ICON global storm-resolving model
A model study investigating the sensitivity of aerosol forcing to the volatilities of semi-volatile organic compounds
Characterization of Brown Carbon absorption in different European environments through source contribution analysis
The impact of uncertainty in black carbon's refractive index on simulated optical depth and radiative forcing
Decomposing the effective radiative forcing of anthropogenic aerosols based on CMIP6 Earth system models
Modeling impacts of dust mineralogy on fast climate response
Uncertainties in laboratory-measured shortwave refractive indices of mineral dust aerosols and derived optical properties: a theoretical assessment
Diagnosing uncertainties in global biomass burning emission inventories and their impact on modeled air pollutants
Role of atmospheric aerosols in severe winter fog over the Indo-Gangetic Plain of India: a case study
Long-term variability in black carbon emissions constrained by gap-filled absorption aerosol optical depth and associated premature mortality in China
Intercomparison of aerosol optical depths from four reanalyses and their multi-reanalysis consensus
Global aviation contrail climate effects from 2019 to 2021
Rapid iodine oxoacid nucleation enhanced by dimethylamine in broad marine regions
Simulations of the impact of cloud condensation nuclei and ice-nucleating particles perturbations on the microphysics and radar reflectivity factor of stratiform mixed-phase clouds
Aerosols in the central Arctic cryosphere: satellite and model integrated insights during Arctic spring and summer
Observationally constrained regional variations of shortwave absorption by iron oxides emphasize the cooling effect of dust
Droplet collection efficiencies inferred from satellite retrievals constrain effective radiative forcing of aerosol–cloud interactions
Global aerosol-type classification using a new hybrid algorithm and Aerosol Robotic Network data
Danny M. Leung, Jasper F. Kok, Longlei Li, David M. Lawrence, Natalie M. Mahowald, Simone Tilmes, and Erik Kluzek
Atmos. Chem. Phys., 25, 2311–2331, https://doi.org/10.5194/acp-25-2311-2025, https://doi.org/10.5194/acp-25-2311-2025, 2025
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This study derives a gridded dust emission dataset for 1841–2000 by employing a combination of observed dust from core records and reanalyzed global dust cycle constraints. We evaluate the ability of global models to replicate the observed historical dust variability by using the emission dataset to force a historical simulation in an Earth system model. We show that prescribing our emissions forces the model to better match observations than other mechanistic models.
Hongyu Liu, Bo Zhang, Richard H. Moore, Luke D. Ziemba, Richard A. Ferrare, Hyundeok Choi, Armin Sorooshian, David Painemal, Hailong Wang, Michael A. Shook, Amy Jo Scarino, Johnathan W. Hair, Ewan C. Crosbie, Marta A. Fenn, Taylor J. Shingler, Chris A. Hostetler, Gao Chen, Mary M. Kleb, Gan Luo, Fangqun Yu, Mark A. Vaughan, Yongxiang Hu, Glenn S. Diskin, John B. Nowak, Joshua P. DiGangi, Yonghoon Choi, Christoph A. Keller, and Matthew S. Johnson
Atmos. Chem. Phys., 25, 2087–2121, https://doi.org/10.5194/acp-25-2087-2025, https://doi.org/10.5194/acp-25-2087-2025, 2025
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We use the GEOS-Chem model to simulate aerosol distributions and properties over the western North Atlantic Ocean (WNAO) during the winter and summer deployments in 2020 of the NASA ACTIVATE mission. Model results are evaluated against aircraft, ground-based, and satellite observations. The improved understanding of life cycle, composition, transport pathways, and distribution of aerosols has important implications for characterizing aerosol–cloud–meteorology interactions over WNAO.
Mingrui Ma, Jiachen Cao, Dan Tong, Bo Zheng, and Yu Zhao
Atmos. Chem. Phys., 25, 2147–2166, https://doi.org/10.5194/acp-25-2147-2025, https://doi.org/10.5194/acp-25-2147-2025, 2025
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We combined two global climate change pathways and three national emission control scenarios to analyze the future evolution of reactive nitrogen (Nr) deposition till the 2060s in China with air quality modeling. We show China’s clean air and carbon neutrality policies would overcome the adverse effects of climate change and efficiently reduce Nr deposition. The outflow of Nr fluxes from mainland China to the west Pacific would also be clearly reduced from continuous stringent emission controls.
Zhouyang Zhang, Jiandong Wang, Jiaping Wang, Nicole Riemer, Chao Liu, Yuzhi Jin, Zeyuan Tian, Jing Cai, Yueyue Cheng, Ganzhen Chen, Bin Wang, Shuxiao Wang, and Aijun Ding
Atmos. Chem. Phys., 25, 1869–1881, https://doi.org/10.5194/acp-25-1869-2025, https://doi.org/10.5194/acp-25-1869-2025, 2025
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Black carbon (BC) exerts notable warming effects. We use a particle-resolved model to investigate the long-term behavior of the BC mixing state, revealing its compositions, coating thickness distribution, and optical properties all stabilize with a characteristic time of less than 1 d. This study can effectively simplify the description of the BC mixing state, which facilitates the precise assessment of the optical properties of BC aerosols in global and chemical transport models.
Qianyi Huo, Zhicong Yin, Xiaoqing Ma, and Huijun Wang
Atmos. Chem. Phys., 25, 1711–1724, https://doi.org/10.5194/acp-25-1711-2025, https://doi.org/10.5194/acp-25-1711-2025, 2025
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Dust days during the spring seasons of 2015–2023 in North China were classified into Mongolian cyclone and cold high types depending on the presence of the Mongolian cyclone. The Mongolian cyclone type led to more frequent and severe dust weather, indicated by PM10 concentrations. To comprehensively forecast the two types of dust weather, a common predictor was established based on 500 hPa anomalous circulation systems, offering insights for dust weather forecasting and climate prediction.
Mariya Petrenko, Ralph Kahn, Mian Chin, Susanne E. Bauer, Tommi Bergman, Huisheng Bian, Gabriele Curci, Ben Johnson, Johannes W. Kaiser, Zak Kipling, Harri Kokkola, Xiaohong Liu, Keren Mezuman, Tero Mielonen, Gunnar Myhre, Xiaohua Pan, Anna Protonotariou, Samuel Remy, Ragnhild Bieltvedt Skeie, Philip Stier, Toshihiko Takemura, Kostas Tsigaridis, Hailong Wang, Duncan Watson-Parris, and Kai Zhang
Atmos. Chem. Phys., 25, 1545–1567, https://doi.org/10.5194/acp-25-1545-2025, https://doi.org/10.5194/acp-25-1545-2025, 2025
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We compared smoke plume simulations from 11 global models to each other and to satellite smoke amount observations aimed at constraining smoke source strength. In regions where plumes are thick and background aerosol is low, models and satellites compare well. However, the input emission inventory tends to underestimate in many places, and particle property and loss rate assumptions vary enormously among models, causing uncertainties that require systematic in situ measurements to resolve.
Yongqing Bai, Tianliang Zhao, Kai Meng, Yue Zhou, Jie Xiong, Xiaoyun Sun, Lijuan Shen, Yanyu Yue, Yan Zhu, Weiyang Hu, and Jingyan Yao
Atmos. Chem. Phys., 25, 1273–1287, https://doi.org/10.5194/acp-25-1273-2025, https://doi.org/10.5194/acp-25-1273-2025, 2025
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We proposed a composite statistical method to identify the quasi-weekly oscillation (QWO) of regional PM2.5 transport over China in winter from 2015 to 2019. The QWO of regional PM2.5 transport is constrained by synoptic-scale disturbances of the East Asian winter monsoon circulation with the periodic activities of the Siberian high, providing a new insight into the understanding of regional pollutant transport with meteorological drivers in atmospheric environment changes.
Léo Clauzel, Sandrine Anquetin, Christophe Lavaysse, Gilles Bergametti, Christel Bouet, Guillaume Siour, Rémy Lapere, Béatrice Marticorena, and Jennie Thomas
Atmos. Chem. Phys., 25, 997–1021, https://doi.org/10.5194/acp-25-997-2025, https://doi.org/10.5194/acp-25-997-2025, 2025
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Solar energy production in West Africa is set to rise and needs accurate solar radiation estimates which are affected by desert dust. This work analyses a March 2021 dust event using a modelling strategy incorporating desert dust. Results show that considering desert dust cuts errors in solar radiation estimates by 75 % and reduces surface solar radiation by 18 %. This highlights the importance of incorporating dust aerosols into solar forecasting for better accuracy.
Ross J. Herbert, Alberto Sanchez-Marroquin, Daniel P. Grosvenor, Kirsty J. Pringle, Stephen R. Arnold, Benjamin J. Murray, and Kenneth S. Carslaw
Atmos. Chem. Phys., 25, 291–325, https://doi.org/10.5194/acp-25-291-2025, https://doi.org/10.5194/acp-25-291-2025, 2025
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Aerosol particles that help form ice in clouds vary in number and type around the world and with time. However, in many weather and climate models cloud ice is not linked to aerosols that are known to nucleate ice. Here we report the first steps towards representing ice-nucleating particles within the UK Earth System Model. We conclude that in addition to ice nucleation by sea spray and mineral components of soil dust, we also need to represent ice nucleation by the organic components of soils.
Ryan Schmedding and Andreas Zuend
Atmos. Chem. Phys., 25, 327–346, https://doi.org/10.5194/acp-25-327-2025, https://doi.org/10.5194/acp-25-327-2025, 2025
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Four different approaches for computing the interfacial tension between liquid phases in aerosol particles were tested for particles with diameters from 10 nm to more than 5 μm. Antonov's rule led to the strongest reductions in the onset relative humidity of liquid–liquid phase separation and reproduced measured interfacial tensions for highly immiscible systems. A modified form of the Butler equation was able to best reproduce measured interfacial tensions in more miscible systems.
Masaru Yoshioka, Daniel P. Grosvenor, Ben B. B. Booth, Colin P. Morice, and Ken S. Carslaw
Atmos. Chem. Phys., 24, 13681–13692, https://doi.org/10.5194/acp-24-13681-2024, https://doi.org/10.5194/acp-24-13681-2024, 2024
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A 2020 regulation has reduced sulfur emissions from shipping by about 80 %, leading to a decrease in atmospheric aerosols that have a cooling effect primarily by affecting cloud properties and amounts. Our climate model simulations predict a global temperature increase of 0.04 K over the next 3 decades as a result, which could contribute to surpassing the Paris Agreement's 1.5 °C target. Reduced aerosols may have also contributed to the recent temperature spikes.
Alcide Zhao, Laura J. Wilcox, and Claire L. Ryder
Atmos. Chem. Phys., 24, 13385–13402, https://doi.org/10.5194/acp-24-13385-2024, https://doi.org/10.5194/acp-24-13385-2024, 2024
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Climate models include desert dust aerosols, which cause atmospheric heating and can change circulation patterns. We assess the effect of dust on the Indian and east Asian summer monsoons through multi-model experiments isolating the effect of dust in current climate models for the first time. Dust atmospheric heating results in a southward shift of western Pacific equatorial rainfall and an enhanced Indian summer monsoon. This shows the importance of accurate dust representation in models.
Ragnhild Bieltvedt Skeie, Rachael Byrom, Øivind Hodnebrog, Caroline Jouan, and Gunnar Myhre
Atmos. Chem. Phys., 24, 13361–13370, https://doi.org/10.5194/acp-24-13361-2024, https://doi.org/10.5194/acp-24-13361-2024, 2024
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In 2020, new regulations by the International Maritime Organization regarding sulfur emissions came into force, reducing emissions of SO2 from the shipping sector by approximately 80 %. In this study, we use multiple models to calculate how much the Earth energy balance changed due to the emission reduction or the so-called effective radiative forcing. The calculated effective radiative forcing is weak, comparable to the effect of the increase in CO2 over the last 2 to 3 years.
Mingxu Liu, Hitoshi Matsui, Douglas S. Hamilton, Sagar D. Rathod, Kara D. Lamb, and Natalie M. Mahowald
Atmos. Chem. Phys., 24, 13115–13127, https://doi.org/10.5194/acp-24-13115-2024, https://doi.org/10.5194/acp-24-13115-2024, 2024
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Atmospheric aerosol deposition provides bioavailable iron to promote marine primary production, yet the estimates of its fluxes remain highly uncertain. This study, by performing global aerosol simulations, demonstrates that iron-containing particle size upon emission is a critical factor in regulating soluble iron input to open oceans. Further observational constraints on this are needed to reduce modeling uncertainties.
Camelia Talianu, Jeni Vasilescu, Doina Nicolae, Alexandru Ilie, Andrei Dandocsi, Anca Nemuc, and Livio Belegante
EGUsphere, https://doi.org/10.5194/egusphere-2024-2930, https://doi.org/10.5194/egusphere-2024-2930, 2024
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Bucharest, Romania's capital, has successfully used mobile measurements and mixed-effects LUR models to derive seasonal maps of near-surface PM10, NO2, and UFP. The data was collected during two intensive campaigns, covering high-traffic streets, residential, industrial, and commercial districts. The model's performance was evaluated, demonstrating its potential for high-resolution mapping in other cities with well-characterized urban structures and diverse in situ monitoring stations.
Jingmin Li, Mattia Righi, Johannes Hendricks, Christof G. Beer, Ulrike Burkhardt, and Anja Schmidt
Atmos. Chem. Phys., 24, 12727–12747, https://doi.org/10.5194/acp-24-12727-2024, https://doi.org/10.5194/acp-24-12727-2024, 2024
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Aiming to understand underlying patterns and trends in aerosols, we characterize the spatial patterns and long-term evolution of lower tropospheric aerosols by clustering multiple aerosol properties from preindustrial times to the year 2050 under three Shared
Socioeconomic Pathway scenarios. The results provide a clear and condensed picture of the spatial extent and distribution of aerosols for different time periods and emission scenarios.
Socioeconomic Pathway scenarios. The results provide a clear and condensed picture of the spatial extent and distribution of aerosols for different time periods and emission scenarios.
Yueming Cheng, Tie Dai, Junji Cao, Daisuke Goto, Jianbing Jin, Teruyuki Nakajima, and Guangyu Shi
Atmos. Chem. Phys., 24, 12643–12659, https://doi.org/10.5194/acp-24-12643-2024, https://doi.org/10.5194/acp-24-12643-2024, 2024
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In March 2021, east Asia experienced an outbreak of severe dust storms after an absence of 1.5 decades. Here, we innovatively used the time-lagged ground-based aerosol size information with the fixed-lag ensemble Kalman smoother to optimize dust emission and reproduce the dust storm. This work is valuable for not only the quantification of health damage, aviation risks, and profound impacts on the Earth's system but also revealing the climatic driving force and the process of desertification.
Marc Mallet, Aurore Voldoire, Fabien Solmon, Pierre Nabat, Thomas Drugé, and Romain Roehrig
Atmos. Chem. Phys., 24, 12509–12535, https://doi.org/10.5194/acp-24-12509-2024, https://doi.org/10.5194/acp-24-12509-2024, 2024
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This study investigates the interactions between smoke aerosols and climate in tropical Africa using a coupled ocean–atmosphere–aerosol climate model. The work shows that smoke plumes have a significant impact by increasing the low-cloud fraction, decreasing the ocean and continental surface temperature and reducing the precipitation of coastal western Africa. It also highlights the role of the ocean temperature response and its feedbacks for the September–November season.
Jia Liu, Cancan Zhu, Donghui Zhou, and Jinbao Han
Atmos. Chem. Phys., 24, 12341–12354, https://doi.org/10.5194/acp-24-12341-2024, https://doi.org/10.5194/acp-24-12341-2024, 2024
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The hydrophilic coatings of aged black carbon (BC) particles absorb moisture during the hygroscopic growth process, but it is difficult to characterize how much water is absorbed under different relative humidities (RHs). In this study, we propose a method to obtain the water content in the coatings based on the equivalent complex refractive index retrieved from optical properties. This method is verified from a theoretical perspective, and it performs well for thickly coated BC at high RHs.
Zijun Li, Angela Buchholz, and Noora Hyttinen
Atmos. Chem. Phys., 24, 11717–11725, https://doi.org/10.5194/acp-24-11717-2024, https://doi.org/10.5194/acp-24-11717-2024, 2024
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Evaluating organosulfur (OS) hygroscopicity is important for assessing aerosol–cloud climate interactions in the post-fossil-fuel future, when SO2 emissions decrease and OS compounds become increasingly important. Here a state-of-the-art quantum-chemistry-based method was used to predict the hygroscopic growth factors (HGFs) of a group of atmospherically relevant OS compounds and their mixtures with (NH4)2SO4. A good agreement was observed between their model-estimated and experimental HGFs.
Jamie R. Banks, Bernd Heinold, and Kerstin Schepanski
Atmos. Chem. Phys., 24, 11451–11475, https://doi.org/10.5194/acp-24-11451-2024, https://doi.org/10.5194/acp-24-11451-2024, 2024
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The Aralkum is a new desert in Central Asia formed by the desiccation of the Aral Sea. This has created a source of atmospheric dust, with implications for the balance of solar and thermal radiation. Simulating these effects using a dust transport model, we find that Aralkum dust adds radiative cooling effects to the surface and atmosphere on average but also adds heating events. Increases in surface pressure due to Aralkum dust strengthen the Siberian High and weaken the summer Asian heat low.
Xinyue Shao, Minghuai Wang, Xinyi Dong, Yaman Liu, Wenxiang Shen, Stephen R. Arnold, Leighton A. Regayre, Meinrat O. Andreae, Mira L. Pöhlker, Duseong S. Jo, Man Yue, and Ken S. Carslaw
Atmos. Chem. Phys., 24, 11365–11389, https://doi.org/10.5194/acp-24-11365-2024, https://doi.org/10.5194/acp-24-11365-2024, 2024
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Highly oxygenated organic molecules (HOMs) play an important role in atmospheric new particle formation (NPF). By semi-explicitly coupling the chemical mechanism of HOMs and a comprehensive nucleation scheme in a global climate model, the updated model shows better agreement with measurements of nucleation rate, growth rate, and NPF event frequency. Our results reveal that HOM-driven NPF leads to a considerable increase in particle and cloud condensation nuclei burden globally.
Falei Xu, Shuang Wang, Yan Li, and Juan Feng
Atmos. Chem. Phys., 24, 10689–10705, https://doi.org/10.5194/acp-24-10689-2024, https://doi.org/10.5194/acp-24-10689-2024, 2024
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This study examines how the winter North Atlantic Oscillation (NAO) and El Niño–Southern Oscillation (ENSO) affect dust activities in North China during the following spring. The results show that the NAO and ENSO, particularly in their negative phases, greatly influence dust activities. When both are negative, their combined effect on dust activities is even greater. This research highlights the importance of these climate patterns in predicting spring dust activities in North China.
Hengheng Zhang, Wei Huang, Xiaoli Shen, Ramakrishna Ramisetty, Junwei Song, Olga Kiseleva, Christopher Claus Holst, Basit Khan, Thomas Leisner, and Harald Saathoff
Atmos. Chem. Phys., 24, 10617–10637, https://doi.org/10.5194/acp-24-10617-2024, https://doi.org/10.5194/acp-24-10617-2024, 2024
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Our study unravels how stagnant winter conditions elevate aerosol levels in Stuttgart. Cloud cover at night plays a pivotal role, impacting morning air quality. Validating a key model, our findings aid accurate air quality predictions, crucial for effective pollution mitigation in urban areas.
Giorgio Veratti, Alessandro Bigi, Michele Stortini, Sergio Teggi, and Grazia Ghermandi
Atmos. Chem. Phys., 24, 10475–10512, https://doi.org/10.5194/acp-24-10475-2024, https://doi.org/10.5194/acp-24-10475-2024, 2024
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In a study of two consecutive winter seasons, we used measurements and modelling tools to identify the levels and sources of black carbon pollution in a medium-sized urban area of the Po Valley, Italy. Our findings show that biomass burning and traffic-related emissions (especially from Euro 4 diesel cars) significantly contribute to BC concentrations. This research offers crucial insights for policymakers and urban planners aiming to improve air quality in cities.
Jiangtao Li, Xingqin An, Zhaobin Sun, Caihua Ye, Qing Hou, Yuxin Zhao, and Zhe Liu
EGUsphere, https://doi.org/10.5194/egusphere-2024-2000, https://doi.org/10.5194/egusphere-2024-2000, 2024
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Climate change and pollution have intensified pollen allergies. We developed a pollen emissions model using phenology and random forests. Key factors affecting annual pollen emissions include temperature, relative humidity, and sunshine hours. Pollen dispersal starts around August 10, peaks around August 30, and ends by September 25, lasting about 45 days. Over time, annual pollen emissions exhibit significant fluctuations and a downward trend.
Pascal Lemaitre, Arnaud Quérel, Alexis Dépée, Alice Guerra Devigne, Marie Monier, Thibault Hiron, Chloé Soto Minguez, Daniel Hardy, and Andrea Flossmann
Atmos. Chem. Phys., 24, 9713–9732, https://doi.org/10.5194/acp-24-9713-2024, https://doi.org/10.5194/acp-24-9713-2024, 2024
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A new in-cloud scavenging scheme is proposed. It is based on a microphysical model of cloud formation and may be applied to long-distance atmospheric transport models (> 100 km) and climatic models. This model is applied to the two most extreme precipitating cloud types in terms of both relative humidity and vertical extension: cumulonimbus and stratus.
Alex Rowell, James Brean, David C. S. Beddows, Tuukka Petäjä, Máté Vörösmarty, Imre Salma, Jarkko V. Niemi, Hanna E. Manninen, Dominik van Pinxteren, Thomas Tuch, Kay Weinhold, Zongbo Shi, and Roy M. Harrison
Atmos. Chem. Phys., 24, 9515–9531, https://doi.org/10.5194/acp-24-9515-2024, https://doi.org/10.5194/acp-24-9515-2024, 2024
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Different sources of airborne particles in the atmospheres of four European cities were distinguished by recognising their particle size distributions using a statistical procedure, positive matrix factorisation. The various sources responded differently to the changes in emissions associated with COVID-19 lockdowns, and the reasons are investigated. While traffic emissions generally decreased, particles formed from reactions of atmospheric gases decreased in some cities but increased in others.
Amy H. Peace, Ying Chen, George Jordan, Daniel G. Partridge, Florent Malavelle, Eliza Duncan, and Jim M. Haywood
Atmos. Chem. Phys., 24, 9533–9553, https://doi.org/10.5194/acp-24-9533-2024, https://doi.org/10.5194/acp-24-9533-2024, 2024
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Natural aerosols from volcanic eruptions can help us understand how anthropogenic aerosols modify climate. We use observations and model simulations of the 2014–2015 Holuhraun eruption plume to examine aerosol–cloud interactions in September 2014. We find a shift to clouds with smaller, more numerous cloud droplets in the first 2 weeks of the eruption. In the third week, the background meteorology and previous conditions experienced by air masses modulate the aerosol perturbation to clouds.
Hua Lu, Min Xie, Bingliang Zhuang, Danyang Ma, Bojun Liu, Yangzhihao Zhan, Tijian Wang, Shu Li, Mengmeng Li, and Kuanguang Zhu
Atmos. Chem. Phys., 24, 8963–8982, https://doi.org/10.5194/acp-24-8963-2024, https://doi.org/10.5194/acp-24-8963-2024, 2024
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To identify cloud, aerosol, and planetary boundary layer (PBL) interactions from an air quality perspective, we summarized two pollution patterns characterized by denser liquid cloud and by obvious cloud radiation interaction (CRI). Numerical simulation experiments showed CRI could cause a 50 % reduction in aerosol radiation interaction (ARI) under a low-trough system. The results emphasized the nonnegligible role of CRI and its inhibition of ARI under wet and cloudy pollution synoptic patterns.
Zhe Song, Ningning Yao, Lang Chen, Yuhai Sun, Boqiong Jiang, Pengfei Li, Daniel Rosenfeld, and Shaocai Yu
EGUsphere, https://doi.org/10.5194/egusphere-2024-2263, https://doi.org/10.5194/egusphere-2024-2263, 2024
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Our results with injected sea-salt aerosols for five open oceans show that the sea-salt aerosols with low injection amounts dominated the shortwave radiation mainly through the indirect effects. As indirect aerosol effects saturated with increasing injection rates, direct effects exceeded indirect effects. This implies that marine cloud brightening was best implemented in areas with extensive cloud cover, while the aerosol direct scattering effects remained dominant when clouds were scarce.
Yuzhi Jin, Jiandong Wang, David C. Wong, Chao Liu, Golam Sarwar, Kathleen M. Fahey, Shang Wu, Jiaping Wang, Jing Cai, Zeyuan Tian, Zhouyang Zhang, Jia Xing, Aijun Ding, and Shuxiao Wang
EGUsphere, https://doi.org/10.5194/egusphere-2024-2372, https://doi.org/10.5194/egusphere-2024-2372, 2024
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Black carbon (BC) affects climate and the environment, and its aging process alters its properties. Current models, like WRF-CMAQ, lack full account. We developed the WRF-CMAQ-BCG model to better represent BC aging by introducing Bare/Coated BC species and their conversion. Our findings show that BC mixing states have distinct spatiotemporal distribution characteristics, and BC wet deposition is dominated by Coated BC. Accounting for BC aging process improves aerosol optics simulation accuracy.
Emilie Fons, Ann Kristin Naumann, David Neubauer, Theresa Lang, and Ulrike Lohmann
Atmos. Chem. Phys., 24, 8653–8675, https://doi.org/10.5194/acp-24-8653-2024, https://doi.org/10.5194/acp-24-8653-2024, 2024
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Aerosols can modify the liquid water path (LWP) of stratocumulus and, thus, their radiative effect. We compare storm-resolving model and satellite data that disagree on the sign of LWP adjustments and diagnose this discrepancy with causal inference. We find that strong precipitation, the absence of wet scavenging, and cloud deepening under a weak inversion contribute to positive LWP adjustments to aerosols in the model, despite weak negative effects from cloud-top entrainment enhancement.
Muhammed Irfan, Thomas Kühn, Taina Yli-Juuti, Anton Laakso, Eemeli Holopainen, Douglas R. Worsnop, Annele Virtanen, and Harri Kokkola
Atmos. Chem. Phys., 24, 8489–8506, https://doi.org/10.5194/acp-24-8489-2024, https://doi.org/10.5194/acp-24-8489-2024, 2024
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The study examines how the volatility of semi-volatile organic compounds affects secondary organic aerosol (SOA) formation and climate. Our simulations show that uncertainties in these volatilities influence aerosol mass and climate impacts. Accurate representation of these compounds in climate models is crucial for predicting global climate patterns.
Hector Navarro-Barboza, Jordi Rovira, Vincenzo Obiso, Andrea Pozzer, Marta Via, Andres Alastuey, Xavier Querol, Noemi Perez, Marjan Savadkoohi, Gang Chen, Jesus Yus-Díez, Matic Ivancic, Martin Rigler, Konstantinos Eleftheriadis, Stergios Vratolis, Olga Zografou, Maria Gini, Benjamin Chazeau, Nicolas Marchand, Andre Prevot, Kaspar Dallenbach, Mikael Ehn, Krista Luoma, Tuukka Petäjä, Anna Tobler, Jaroslaw Necki, Minna Aurela, Hilkka Timonen, Jarkko Niemi, Olivier Favez, Jean-Eudes Petit, Jean-Philippe Putaud, Christoph Hueglin, Nicolas Pascal, Aurelien Chauvigné, Sebastien Conil, Marco Pandolfi, and Oriol Jorba
EGUsphere, https://doi.org/10.5194/egusphere-2024-2086, https://doi.org/10.5194/egusphere-2024-2086, 2024
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Brown carbon (BrC) absorbs UV and visible light, affecting climate. Our study investigates BrC's imaginary refractive index (k ) using data from 12 European sites. Residential emissions are a major OA source in winter, while secondary organic aerosols (SOA) dominate in summer. We derived source-specific k values, enhancing model accuracy. This research improves understanding of BrC's climate role, emphasizing the need for source-specific constraints in atmospheric models.
Ruth A. R. Digby, Knut von Salzen, Adam H. Monahan, Nathan P. Gillett, and Jiangnan Li
EGUsphere, https://doi.org/10.5194/egusphere-2024-1796, https://doi.org/10.5194/egusphere-2024-1796, 2024
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The refractive index of black carbon (BCRI), which determines how much energy black carbon absorbs and scatters, is difficult to measure and different climate models use different values. We show that varying the BCRI across commonly used values can increase absorbing aerosol optical depth by 42 % and the warming effect from interactions between black carbon and radiation by 47 %, an appreciable fraction of the overall spread between models reported in recent literature assessments.
Alkiviadis Kalisoras, Aristeidis K. Georgoulias, Dimitris Akritidis, Robert J. Allen, Vaishali Naik, Chaincy Kuo, Sophie Szopa, Pierre Nabat, Dirk Olivié, Twan van Noije, Philippe Le Sager, David Neubauer, Naga Oshima, Jane Mulcahy, Larry W. Horowitz, and Prodromos Zanis
Atmos. Chem. Phys., 24, 7837–7872, https://doi.org/10.5194/acp-24-7837-2024, https://doi.org/10.5194/acp-24-7837-2024, 2024
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Effective radiative forcing (ERF) is a metric for estimating how human activities and natural agents change the energy flow into and out of the Earth’s climate system. We investigate the anthropogenic aerosol ERF, and we estimate the contribution of individual processes to the total ERF using simulations from Earth system models within the Coupled Model Intercomparison Project Phase 6 (CMIP6). Our findings highlight that aerosol–cloud interactions drive ERF variability during the last 150 years.
Qianqian Song, Paul Ginoux, María Gonçalves Ageitos, Ron L. Miller, Vincenzo Obiso, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 7421–7446, https://doi.org/10.5194/acp-24-7421-2024, https://doi.org/10.5194/acp-24-7421-2024, 2024
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We implement and simulate the distribution of eight dust minerals in the GFDL AM4.0 model. We found that resolving the eight minerals reduces dust absorption compared to the homogeneous dust used in the standard GFDL AM4.0 model that assumes a globally uniform hematite content of 2.7 % by volume. Resolving dust mineralogy results in significant impacts on radiation, land surface temperature, surface winds, and precipitation over North Africa in summer.
Senyi Kong, Zheng Wang, and Lei Bi
Atmos. Chem. Phys., 24, 6911–6935, https://doi.org/10.5194/acp-24-6911-2024, https://doi.org/10.5194/acp-24-6911-2024, 2024
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The retrieval of refractive indices of dust aerosols from laboratory optical measurements is commonly done assuming spherical particles. This paper aims to investigate the uncertainties in the shortwave refractive indices and corresponding optical properties by considering non-spherical and inhomogeneous models for dust samples. The study emphasizes the significance of using non-spherical models for simulating dust aerosols.
Wenxuan Hua, Sijia Lou, Xin Huang, Lian Xue, Ke Ding, Zilin Wang, and Aijun Ding
Atmos. Chem. Phys., 24, 6787–6807, https://doi.org/10.5194/acp-24-6787-2024, https://doi.org/10.5194/acp-24-6787-2024, 2024
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In this study, we diagnose uncertainties in carbon monoxide and organic carbon emissions from four inventories for seven major wildfire-prone regions. Uncertainties in vegetation classification methods, fire detection products, and cloud obscuration effects lead to bias in these biomass burning (BB) emission inventories. By comparing simulations with measurements, we provide certain inventory recommendations. Our study has implications for reducing uncertainties in emissions in further studies.
Chandrakala Bharali, Mary Barth, Rajesh Kumar, Sachin D. Ghude, Vinayak Sinha, and Baerbel Sinha
Atmos. Chem. Phys., 24, 6635–6662, https://doi.org/10.5194/acp-24-6635-2024, https://doi.org/10.5194/acp-24-6635-2024, 2024
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This study examines the role of atmospheric aerosols in winter fog over the Indo-Gangetic Plains of India using WRF-Chem. The increase in RH with aerosol–radiation feedback (ARF) is found to be important for fog formation as it promotes the growth of aerosols in the polluted environment. Aqueous-phase chemistry in the fog increases PM2.5 concentration, further affecting ARF. ARF and aqueous-phase chemistry affect the fog intensity and the timing of fog formation by ~1–2 h.
Wenxin Zhao, Yu Zhao, Yu Zheng, Dong Chen, Jinyuan Xin, Kaitao Li, Huizheng Che, Zhengqiang Li, Mingrui Ma, and Yun Hang
Atmos. Chem. Phys., 24, 6593–6612, https://doi.org/10.5194/acp-24-6593-2024, https://doi.org/10.5194/acp-24-6593-2024, 2024
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We evaluate the long-term (2000–2020) variabilities of aerosol absorption optical depth, black carbon emissions, and associated health risks in China with an integrated framework that combines multiple observations and modeling techniques. We demonstrate the remarkable emission abatement resulting from the implementation of national pollution controls and show how human activities affected the emissions with a spatiotemporal heterogeneity, thus supporting differentiated policy-making by region.
Peng Xian, Jeffrey S. Reid, Melanie Ades, Angela Benedetti, Peter R. Colarco, Arlindo da Silva, Tom F. Eck, Johannes Flemming, Edward J. Hyer, Zak Kipling, Samuel Rémy, Tsuyoshi Thomas Sekiyama, Taichu Tanaka, Keiya Yumimoto, and Jianglong Zhang
Atmos. Chem. Phys., 24, 6385–6411, https://doi.org/10.5194/acp-24-6385-2024, https://doi.org/10.5194/acp-24-6385-2024, 2024
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The study compares and evaluates monthly AOD of four reanalyses (RA) and their consensus (i.e., ensemble mean). The basic verification characteristics of these RA versus both AERONET and MODIS retrievals are presented. The study discusses the strength of each RA and identifies regions where divergence and challenges are prominent. The RA consensus usually performs very well on a global scale in terms of how well it matches the observational data, making it a good choice for various applications.
Roger Teoh, Zebediah Engberg, Ulrich Schumann, Christiane Voigt, Marc Shapiro, Susanne Rohs, and Marc E. J. Stettler
Atmos. Chem. Phys., 24, 6071–6093, https://doi.org/10.5194/acp-24-6071-2024, https://doi.org/10.5194/acp-24-6071-2024, 2024
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The radiative forcing (RF) due to aviation contrails is comparable to that caused by CO2. We estimate that global contrail net RF in 2019 was 62.1 mW m−2. This is ~1/2 the previous best estimate for 2018. Contrail RF varies regionally due to differences in conditions required for persistent contrails. COVID-19 reduced contrail RF by 54% in 2020 relative to 2019. Globally, 2 % of all flights account for 80 % of the annual contrail energy forcing, suggesting a opportunity to mitigate contrail RF.
Haotian Zu, Biwu Chu, Yiqun Lu, Ling Liu, and Xiuhui Zhang
Atmos. Chem. Phys., 24, 5823–5835, https://doi.org/10.5194/acp-24-5823-2024, https://doi.org/10.5194/acp-24-5823-2024, 2024
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The nucleation of iodic acid (HIO3) and iodous acid (HIO2) was proven to be critical in marine areas. However, HIO3–HIO2 nucleation cannot effectively derive the rapid nucleation in some polluted coasts. We find a significant enhancement of dimethylamine (DMA) on the HIO3–HIO2 nucleation in marine and polar regions with abundant DMA sources, which may establish reasonable connections between the HIO3–HIO2 nucleation and the rapid formation of new particles in polluted marine and polar regions.
Junghwa Lee, Patric Seifert, Tempei Hashino, Maximilian Maahn, Fabian Senf, and Oswald Knoth
Atmos. Chem. Phys., 24, 5737–5756, https://doi.org/10.5194/acp-24-5737-2024, https://doi.org/10.5194/acp-24-5737-2024, 2024
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Spectral bin model simulations of an idealized supercooled stratiform cloud were performed with the AMPS model for variable CCN and INP concentrations. We performed radar forward simulations with PAMTRA to transfer the simulations into radar observational space. The derived radar reflectivity factors were compared to observational studies of stratiform mixed-phase clouds. These studies report a similar response of the radar reflectivity factor to aerosol perturbations as we found in our study.
Basudev Swain, Marco Vountas, Aishwarya Singh, Nidhi L. Anchan, Adrien Deroubaix, Luca Lelli, Yanick Ziegler, Sachin S. Gunthe, Hartmut Bösch, and John P. Burrows
Atmos. Chem. Phys., 24, 5671–5693, https://doi.org/10.5194/acp-24-5671-2024, https://doi.org/10.5194/acp-24-5671-2024, 2024
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Arctic amplification (AA) accelerates the warming of the central Arctic cryosphere and affects aerosol dynamics. Limited observations hinder a comprehensive analysis. This study uses AEROSNOW aerosol optical density (AOD) data and GEOS-Chem simulations to assess AOD variability. Discrepancies highlight the need for improved observational integration into models to refine our understanding of aerosol effects on cloud microphysics, ice nucleation, and radiative forcing under evolving AA.
Vincenzo Obiso, María Gonçalves Ageitos, Carlos Pérez García-Pando, Jan P. Perlwitz, Gregory L. Schuster, Susanne E. Bauer, Claudia Di Biagio, Paola Formenti, Kostas Tsigaridis, and Ron L. Miller
Atmos. Chem. Phys., 24, 5337–5367, https://doi.org/10.5194/acp-24-5337-2024, https://doi.org/10.5194/acp-24-5337-2024, 2024
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We calculate the dust direct radiative effect (DRE) in an Earth system model accounting for regionally varying soil mineralogy through a new observationally constrained method. Linking dust absorption at solar wavelengths to the varying amount of specific minerals (i.e., iron oxides) improves the modeled range of dust single scattering albedo compared to observations and increases the global cooling by dust. Our results may contribute to improved estimates of the dust DRE and its climate impact.
Charlotte M. Beall, Po-Lun Ma, Matthew W. Christensen, Johannes Mülmenstädt, Adam Varble, Kentaroh Suzuki, and Takuro Michibata
Atmos. Chem. Phys., 24, 5287–5302, https://doi.org/10.5194/acp-24-5287-2024, https://doi.org/10.5194/acp-24-5287-2024, 2024
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Single-layer warm liquid clouds cover nearly one-third of the Earth's surface, and uncertainties regarding the impact of aerosols on their radiative properties pose a significant challenge to climate prediction. Here, we demonstrate how satellite observations can be used to constrain Earth system model estimates of the radiative forcing from the interactions of aerosols with clouds due to warm rain processes.
Xiaoli Wei, Qian Cui, Leiming Ma, Feng Zhang, Wenwen Li, and Peng Liu
Atmos. Chem. Phys., 24, 5025–5045, https://doi.org/10.5194/acp-24-5025-2024, https://doi.org/10.5194/acp-24-5025-2024, 2024
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A new aerosol-type classification algorithm has been proposed. It includes an optical database built by Mie scattering and a complex refractive index working as a baseline to identify different aerosol types. The new algorithm shows high accuracy and efficiency. Hence, a global map of aerosol types was generated to characterize aerosol types across the five continents. It will help improve the accuracy of aerosol inversion and determine the sources of aerosol pollution.
Cited articles
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Kulmala, M., Kerminen, V.-M., Petäjä, T., Ding, A. J., and Wang, L.: Atmospheric gas-to-particle conversion: why NPF events are observed in megacities?, Faraday Discuss., 200, 271–288, https://doi.org/10.1039/C6FD00257A, 2017. a, b, c
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Pierce, J. R., Leaitch, W. R., Liggio, J., Westervelt, D. M., Wainwright, C. D., Abbatt, J. P. D., Ahlm, L., Al-Basheer, W., Cziczo, D. J., Hayden, K. L., Lee, A. K. Y., Li, S.-M., Russell, L. M., Sjostedt, S. J., Strawbridge, K. B., Travis, M., Vlasenko, A., Wentzell, J. J. B., Wiebe, H. A., Wong, J. P. S., and Macdonald, A. M.: Nucleation and condensational growth to CCN sizes during a sustained pristine biogenic SOA event in a forested mountain valley, Atmos. Chem. Phys., 12, 3147–3163, https://doi.org/10.5194/acp-12-3147-2012, 2012. a
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Short summary
In this technical note, we show that the limit of the coagulation scavenging enhancement of charged particles is asymptotically 2; that is, at the limit, charged particles are lost at twice the rate of their neutral counterparts. This has serious implications for aerosol particle survivability where ions play a role in nucleation and growth. Such cases can happen readily in experiments and cannot be neglected in the atmosphere.
In this technical note, we show that the limit of the coagulation scavenging enhancement of...
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