Articles | Volume 19, issue 21
https://doi.org/10.5194/acp-19-13355-2019
© Author(s) 2019. 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-19-13355-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
30 Oct 2019
Research article |
| 30 Oct 2019
| 30 Oct 2019
Rate enhancement in collisions of sulfuric acid molecules due to long-range intermolecular forces
Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, P.O. Box 64, 00014, Helsinki, Finland
Evgeni Zapadinsky
Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, P.O. Box 64, 00014, Helsinki, Finland
Theo Kurtén
Institute for Atmospheric and Earth System Research/Chemistry, Faculty of Science, University of Helsinki, P.O. Box 55, 00014, Helsinki, Finland
Hanna Vehkamäki
Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, P.O. Box 64, 00014, Helsinki, Finland
Bernhard Reischl
Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, P.O. Box 64, 00014, Helsinki, Finland
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Ivo Neefjes, Roope Halonen, Hanna Vehkamäki, and Bernhard Reischl
Atmos. Chem. Phys., 22, 11155–11172, https://doi.org/10.5194/acp-22-11155-2022, https://doi.org/10.5194/acp-22-11155-2022, 2022
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Collisions between ionic and dipolar molecules and clusters facilitate the formation of atmospheric aerosol particles, which affect global climate and air quality. We compared often-used classical approaches for calculating ion–dipole collision rates with robust atomistic computer simulations. While classical approaches work for simple ions and dipoles only, our modeling approach can also efficiently calculate reasonable collision properties for more complex systems.
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
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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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.
Lauri Franzon, Marie Camredon, Richard Valorso, Bernard Aumont, and Theo Kurtén
Atmos. Chem. Phys., 24, 11679–11699, https://doi.org/10.5194/acp-24-11679-2024, https://doi.org/10.5194/acp-24-11679-2024, 2024
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In this article we investigate the formation of large, sticky molecules from various organic compounds entering the atmosphere as primary emissions and the degree to which these processes may contribute to organic aerosol particle mass. More specifically, we qualitatively investigate a recently discovered chemical reaction channel for one of the most important short-lived radical compounds, peroxy radicals, and discover which of these reactions are most atmospherically important.
Lukas Pichelstorfer, Pontus Roldin, Matti Rissanen, Noora Hyttinen, Olga Garmash, Carlton Xavier, Putian Zhou, Petri Clusius, Benjamin Foreback, Thomas Golin Almeida, Chenjuan Deng, Metin Baykara, Theo Kurten, and Michael Boy
EGUsphere, https://doi.org/10.5194/egusphere-2023-1415, https://doi.org/10.5194/egusphere-2023-1415, 2023
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Secondary organic aerosols (SOA) form effectively from gaseous precursors via a process called autoxidation. While key chemical reaction types seem to be known, no general description of autoxidation chemistry exists. In the present work, we present a method to create autoxidation chemistry schemes for any atmospherically relevant hydrocarbon. We exemplarily investigate benzene and its potential to form aerosols. We found that autoxidation, under some conditions, can dominate the SOA formation.
Huan Yang, Ivo Neefjes, Valtteri Tikkanen, Jakub Kubečka, Theo Kurtén, Hanna Vehkamäki, and Bernhard Reischl
Atmos. Chem. Phys., 23, 5993–6009, https://doi.org/10.5194/acp-23-5993-2023, https://doi.org/10.5194/acp-23-5993-2023, 2023
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We present a new analytical model for collision rates between molecules and clusters of arbitrary sizes, accounting for long-range interactions. The model is verified against atomistic simulations of typical acid–base clusters participating in atmospheric new particle formation (NPF). Compared to non-interacting models, accounting for long-range interactions leads to 2–3 times higher collision rates for small clusters, indicating the necessity of including such interactions in NPF modeling.
Melissa Meder, Otso Peräkylä, Jonathan G. Varelas, Jingyi Luo, Runlong Cai, Yanjun Zhang, Theo Kurtén, Matthieu Riva, Matti Rissanen, Franz M. Geiger, Regan J. Thomson, and Mikael Ehn
Atmos. Chem. Phys., 23, 4373–4390, https://doi.org/10.5194/acp-23-4373-2023, https://doi.org/10.5194/acp-23-4373-2023, 2023
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We discuss and show the viability of a method where multiple isotopically labelled precursors are used for probing the formation pathways of highly oxygenated organic molecules (HOMs) from the oxidation of the monoterpene a-pinene. HOMs are very important for secondary organic aerosol (SOA) formation in forested regions, and monoterpenes are the single largest source of SOA globally. The fast reactions forming HOMs have thus far remained elusive despite considerable efforts over the last decade.
Ivo Neefjes, Roope Halonen, Hanna Vehkamäki, and Bernhard Reischl
Atmos. Chem. Phys., 22, 11155–11172, https://doi.org/10.5194/acp-22-11155-2022, https://doi.org/10.5194/acp-22-11155-2022, 2022
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Collisions between ionic and dipolar molecules and clusters facilitate the formation of atmospheric aerosol particles, which affect global climate and air quality. We compared often-used classical approaches for calculating ion–dipole collision rates with robust atomistic computer simulations. While classical approaches work for simple ions and dipoles only, our modeling approach can also efficiently calculate reasonable collision properties for more complex systems.
Golnaz Roudsari, Olli H. Pakarinen, Bernhard Reischl, and Hanna Vehkamäki
Atmos. Chem. Phys., 22, 10099–10114, https://doi.org/10.5194/acp-22-10099-2022, https://doi.org/10.5194/acp-22-10099-2022, 2022
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We use atomistic simulations to study heterogeneous ice nucleation on silver iodide surfaces in slit and wedge geometries at low supercooling which serve as a model of irregularities on real atmospheric aerosol particle surfaces. The revealed microscopic ice nucleation mechanisms in confined geometries strongly support the experimental evidence for the importance of surface features such as cracks or pits functioning as active sites for ice nucleation in the atmosphere.
Haiyan Li, Thomas Golin Almeida, Yuanyuan Luo, Jian Zhao, Brett B. Palm, Christopher D. Daub, Wei Huang, Claudia Mohr, Jordan E. Krechmer, Theo Kurtén, and Mikael Ehn
Atmos. Meas. Tech., 15, 1811–1827, https://doi.org/10.5194/amt-15-1811-2022, https://doi.org/10.5194/amt-15-1811-2022, 2022
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This work evaluated the potential for PTR-based mass spectrometers to detect ROOR and ROOH peroxides both experimentally and through computations. Laboratory experiments using a Vocus PTR observed only noisy signals of potential dimers during α-pinene ozonolysis and a few small signals of dimeric compounds during cyclohexene ozonolysis. Quantum chemical calculations for model ROOR and ROOH systems showed that most of these peroxides should fragment partially following protonation.
Dina Alfaouri, Monica Passananti, Tommaso Zanca, Lauri Ahonen, Juha Kangasluoma, Jakub Kubečka, Nanna Myllys, and Hanna Vehkamäki
Atmos. Meas. Tech., 15, 11–19, https://doi.org/10.5194/amt-15-11-2022, https://doi.org/10.5194/amt-15-11-2022, 2022
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To study what is happening in the atmosphere, it is important to be able to measure the molecules and clusters present in it. In our work, we studied an artifact that happens inside a mass spectrometer, in particular the fragmentation of clusters. We were able to quantify the fragmentation and retrieve the correct concentration and composition of the clusters using our dual (experimental and theoretical) approach.
Shahzad Gani, Lukas Kohl, Rima Baalbaki, Federico Bianchi, Taina M. Ruuskanen, Olli-Pekka Siira, Pauli Paasonen, and Hanna Vehkamäki
Geosci. Commun., 4, 507–516, https://doi.org/10.5194/gc-4-507-2021, https://doi.org/10.5194/gc-4-507-2021, 2021
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In this article, we present authorship guidelines which also include a novel authorship form along with the documentation of the formulation process for a multidisciplinary and interdisciplinary center with more than 250 researchers. Our practical approach promotes fair authorship practices and, by focusing on clear, transparent, and timely communication, helps avoid late-stage authorship conflict.
Emma Lumiaro, Milica Todorović, Theo Kurten, Hanna Vehkamäki, and Patrick Rinke
Atmos. Chem. Phys., 21, 13227–13246, https://doi.org/10.5194/acp-21-13227-2021, https://doi.org/10.5194/acp-21-13227-2021, 2021
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The study of climate change relies on climate models, which require an understanding of aerosol formation. We train a machine-learning model to predict the partitioning coefficients of atmospheric molecules, which govern condensation into aerosols. The model can make instant predictions based on molecular structures with accuracy surpassing that of standard computational methods. This will allow the screening of low-volatility molecules that contribute most to aerosol formation.
Xiaolong Fan, Jing Cai, Chao Yan, Jian Zhao, Yishuo Guo, Chang Li, Kaspar R. Dällenbach, Feixue Zheng, Zhuohui Lin, Biwu Chu, Yonghong Wang, Lubna Dada, Qiaozhi Zha, Wei Du, Jenni Kontkanen, Theo Kurtén, Siddhart Iyer, Joni T. Kujansuu, Tuukka Petäjä, Douglas R. Worsnop, Veli-Matti Kerminen, Yongchun Liu, Federico Bianchi, Yee Jun Tham, Lei Yao, and Markku Kulmala
Atmos. Chem. Phys., 21, 11437–11452, https://doi.org/10.5194/acp-21-11437-2021, https://doi.org/10.5194/acp-21-11437-2021, 2021
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We observed significant concentrations of gaseous HBr and HCl throughout the winter and springtime in urban Beijing, China. Our results indicate that gaseous HCl and HBr are most likely originated from anthropogenic emissions such as burning activities, and the gas–aerosol partitioning may play a crucial role in contributing to the gaseous HCl and HBr. These observations suggest that there is an important recycling pathway of halogen species in inland megacities.
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.
Georgia Michailoudi, Jack J. Lin, Hayato Yuzawa, Masanari Nagasaka, Marko Huttula, Nobuhiro Kosugi, Theo Kurtén, Minna Patanen, and Nønne L. Prisle
Atmos. Chem. Phys., 21, 2881–2894, https://doi.org/10.5194/acp-21-2881-2021, https://doi.org/10.5194/acp-21-2881-2021, 2021
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This study provides insight into hydration of two significant atmospheric compounds, glyoxal and methylglyoxal. Using synchrotron radiation excited X-ray absorption spectroscopy, we confirm that glyoxal is fully hydrated in water, and for the first time, we experimentally detect enol structures in aqueous methylglyoxal. Our results support the contribution of these compounds to secondary organic aerosol formation, known to have a large uncertainty in atmospheric models and climate predictions.
Anna Shcherbacheva, Tracey Balehowsky, Jakub Kubečka, Tinja Olenius, Tapio Helin, Heikki Haario, Marko Laine, Theo Kurtén, and Hanna Vehkamäki
Atmos. Chem. Phys., 20, 15867–15906, https://doi.org/10.5194/acp-20-15867-2020, https://doi.org/10.5194/acp-20-15867-2020, 2020
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Atmospheric new particle formation and cluster growth to aerosol particles is an important field of research, in particular due to the climate change phenomenon. Evaporation rates are very difficult to account for but they are important to explain the formation and growth of particles. Different quantum chemistry (QC) methods produce substantially different values for the evaporation rates. We propose a novel approach for inferring evaporation rates of clusters from available measurements.
Noora Hyttinen, Reyhaneh Heshmatnezhad, Jonas Elm, Theo Kurtén, and Nønne L. Prisle
Atmos. Chem. Phys., 20, 13131–13143, https://doi.org/10.5194/acp-20-13131-2020, https://doi.org/10.5194/acp-20-13131-2020, 2020
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We present aqueous solubilities and activity coefficients of mono- and dicarboxylic acids (C1–C6 and C2–C8, respectively) estimated using the COSMOtherm program. In addition, we have calculated effective equilibrium constants of dimerization and hydration of the same acids in the condensed phase. We were also able to improve the agreement between experimental and estimated properties of monocarboxylic acids in aqueous solutions by including clustering reactions in COSMOtherm calculations.
Tommaso Zanca, Jakub Kubečka, Evgeni Zapadinsky, Monica Passananti, Theo Kurtén, and Hanna Vehkamäki
Atmos. Meas. Tech., 13, 3581–3593, https://doi.org/10.5194/amt-13-3581-2020, https://doi.org/10.5194/amt-13-3581-2020, 2020
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In this paper we quantify (using a statistical model) the probability of decomposition of a representative class of HOM clusters in an APi-TOF mass spectrometer. This is important because it quantifies the systematic error of measurements in a APi-TOF MS due to cluster decomposition. The results (specific for our selected clusters) show that decomposition is negligible, provided their bonding energy is large enough to allow formation in the atmosphere in the first place.
Emma L. D'Ambro, Siegfried Schobesberger, Cassandra J. Gaston, Felipe D. Lopez-Hilfiker, Ben H. Lee, Jiumeng Liu, Alla Zelenyuk, David Bell, Christopher D. Cappa, Taylor Helgestad, Ziyue Li, Alex Guenther, Jian Wang, Matthew Wise, Ryan Caylor, Jason D. Surratt, Theran Riedel, Noora Hyttinen, Vili-Taneli Salo, Galib Hasan, Theo Kurtén, John E. Shilling, and Joel A. Thornton
Atmos. Chem. Phys., 19, 11253–11265, https://doi.org/10.5194/acp-19-11253-2019, https://doi.org/10.5194/acp-19-11253-2019, 2019
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Isoprene is the most abundantly emitted reactive organic gas globally, and thus it is important to understand its fate and role in aerosol formation and growth. A major product of its oxidation is an epoxydiol, IEPOX, which can be efficiently taken up by acidic aerosol to generate substantial amounts of secondary organic aerosol (SOA). We present chamber experiments exploring the properties of IEPOX SOA and reconcile discrepancies between field, laboratory, and model studies of this process.
Theo Kurtén, Noora Hyttinen, Emma Louise D'Ambro, Joel Thornton, and Nønne Lyng Prisle
Atmos. Chem. Phys., 18, 17589–17600, https://doi.org/10.5194/acp-18-17589-2018, https://doi.org/10.5194/acp-18-17589-2018, 2018
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We use COSMO-RS to compute saturation vapor pressures for two products of isoprene photo-oxidation and compare the results to measurements. COSMO-RS is an attractive option for calculating properties of molecules, as it is based on quantum mechanics and requires few fitting parameters. However, we show that the default implementation of this method suffers from errors related to both conformational sampling and intramolecular hydrogen bonding. We propose solutions to these problems.
Ulrich K. Krieger, Franziska Siegrist, Claudia Marcolli, Eva U. Emanuelsson, Freya M. Gøbel, Merete Bilde, Aleksandra Marsh, Jonathan P. Reid, Andrew J. Huisman, Ilona Riipinen, Noora Hyttinen, Nanna Myllys, Theo Kurtén, Thomas Bannan, Carl J. Percival, and David Topping
Atmos. Meas. Tech., 11, 49–63, https://doi.org/10.5194/amt-11-49-2018, https://doi.org/10.5194/amt-11-49-2018, 2018
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Vapor pressures of low-volatility organic molecules at atmospheric temperatures reported in the literature often differ by several orders of magnitude between measurement techniques. These discrepancies exceed the stated uncertainty of each technique, which is generally reported to be smaller than a factor of 2. We determined saturation vapor pressures for the homologous series of polyethylene glycols ranging in vapor pressure at 298 K from 1E−7 Pa to 5E−2 Pa as a reference set.
Emilie Öström, Zhou Putian, Guy Schurgers, Mikhail Mishurov, Niku Kivekäs, Heikki Lihavainen, Mikael Ehn, Matti P. Rissanen, Theo Kurtén, Michael Boy, Erik Swietlicki, and Pontus Roldin
Atmos. Chem. Phys., 17, 8887–8901, https://doi.org/10.5194/acp-17-8887-2017, https://doi.org/10.5194/acp-17-8887-2017, 2017
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We used a model to study how biogenic volatile organic compounds (BVOCs) emitted from the boreal forest contribute to the formation and growth of particles in the atmosphere. Some of these particles are important climate forcers, acting as seeds for cloud droplet fomation. We implemented a new gas chemistry mechanism that describes how the BVOCs are oxidized and form low-volatility highly oxidized organic molecules. With the new mechanism we are able to accurately predict the particle growth.
Hanna K. Lappalainen, Veli-Matti Kerminen, Tuukka Petäjä, Theo Kurten, Aleksander Baklanov, Anatoly Shvidenko, Jaana Bäck, Timo Vihma, Pavel Alekseychik, Meinrat O. Andreae, Stephen R. Arnold, Mikhail Arshinov, Eija Asmi, Boris Belan, Leonid Bobylev, Sergey Chalov, Yafang Cheng, Natalia Chubarova, Gerrit de Leeuw, Aijun Ding, Sergey Dobrolyubov, Sergei Dubtsov, Egor Dyukarev, Nikolai Elansky, Kostas Eleftheriadis, Igor Esau, Nikolay Filatov, Mikhail Flint, Congbin Fu, Olga Glezer, Aleksander Gliko, Martin Heimann, Albert A. M. Holtslag, Urmas Hõrrak, Juha Janhunen, Sirkku Juhola, Leena Järvi, Heikki Järvinen, Anna Kanukhina, Pavel Konstantinov, Vladimir Kotlyakov, Antti-Jussi Kieloaho, Alexander S. Komarov, Joni Kujansuu, Ilmo Kukkonen, Ella-Maria Duplissy, Ari Laaksonen, Tuomas Laurila, Heikki Lihavainen, Alexander Lisitzin, Alexsander Mahura, Alexander Makshtas, Evgeny Mareev, Stephany Mazon, Dmitry Matishov, Vladimir Melnikov, Eugene Mikhailov, Dmitri Moisseev, Robert Nigmatulin, Steffen M. Noe, Anne Ojala, Mari Pihlatie, Olga Popovicheva, Jukka Pumpanen, Tatjana Regerand, Irina Repina, Aleksei Shcherbinin, Vladimir Shevchenko, Mikko Sipilä, Andrey Skorokhod, Dominick V. Spracklen, Hang Su, Dmitry A. Subetto, Junying Sun, Arkady Y. Terzhevik, Yuri Timofeyev, Yuliya Troitskaya, Veli-Pekka Tynkkynen, Viacheslav I. Kharuk, Nina Zaytseva, Jiahua Zhang, Yrjö Viisanen, Timo Vesala, Pertti Hari, Hans Christen Hansson, Gennady G. Matvienko, Nikolai S. Kasimov, Huadong Guo, Valery Bondur, Sergej Zilitinkevich, and Markku Kulmala
Atmos. Chem. Phys., 16, 14421–14461, https://doi.org/10.5194/acp-16-14421-2016, https://doi.org/10.5194/acp-16-14421-2016, 2016
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After kick off in 2012, the Pan-Eurasian Experiment (PEEX) program has expanded fast and today the multi-disciplinary research community covers ca. 80 institutes and a network of ca. 500 scientists from Europe, Russia, and China. Here we introduce scientific topics relevant in this context. This is one of the first multi-disciplinary overviews crossing scientific boundaries, from atmospheric sciences to socio-economics and social sciences.
Elham Baranizadeh, Benjamin N. Murphy, Jan Julin, Saeed Falahat, Carly L. Reddington, Antti Arola, Lars Ahlm, Santtu Mikkonen, Christos Fountoukis, David Patoulias, Andreas Minikin, Thomas Hamburger, Ari Laaksonen, Spyros N. Pandis, Hanna Vehkamäki, Kari E. J. Lehtinen, and Ilona Riipinen
Geosci. Model Dev., 9, 2741–2754, https://doi.org/10.5194/gmd-9-2741-2016, https://doi.org/10.5194/gmd-9-2741-2016, 2016
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The molecular mechanisms through which new ultrafine (< 100 nm) aerosol particles are formed in the atmosphere have puzzled the scientific community for decades. In the past few years, however, significant progress has been made in unraveling these processes through laboratory studies and computational efforts. In this work we have implemented these new developments to an air quality model and study the implications of anthropogenically driven particle formation for European air quality.
Jenni Kontkanen, Tinja Olenius, Katrianne Lehtipalo, Hanna Vehkamäki, Markku Kulmala, and Kari E. J. Lehtinen
Atmos. Chem. Phys., 16, 5545–5560, https://doi.org/10.5194/acp-16-5545-2016, https://doi.org/10.5194/acp-16-5545-2016, 2016
Felipe D. Lopez-Hilfiker, Siddarth Iyer, Claudia Mohr, Ben H. Lee, Emma L. D'Ambro, Theo Kurtén, and Joel A. Thornton
Atmos. Meas. Tech., 9, 1505–1512, https://doi.org/10.5194/amt-9-1505-2016, https://doi.org/10.5194/amt-9-1505-2016, 2016
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We present the maximum sensitivity of a TOF-CIMS using the collision limit and iodide adducts. We also present an ion adduct declustering scanning procedure which determines the effective binding energies of the detected ion adducts and therefore their approximate sensitivity. The combination of declustering scanning and the collision limit provides an approximate calibration for many compounds in the mass spectrum which would otherwise be impossible to obtain by traditional methods.
M. Kulmala, H. K. Lappalainen, T. Petäjä, T. Kurten, V.-M. Kerminen, Y. Viisanen, P. Hari, S. Sorvari, J. Bäck, V. Bondur, N. Kasimov, V. Kotlyakov, G. Matvienko, A. Baklanov, H. D. Guo, A. Ding, H.-C. Hansson, and S. Zilitinkevich
Atmos. Chem. Phys., 15, 13085–13096, https://doi.org/10.5194/acp-15-13085-2015, https://doi.org/10.5194/acp-15-13085-2015, 2015
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The Pan-European Experiment (PEEX) is introduced. PEEX is a multidisciplinary, multiscale and multicomponent research, research infrastructure and capacity-building program. This paper outlines the mission, vision and objectives of PEEX and introduces its main components, including the research agenda, research infrastructure, knowledge transfer and potential impacts on society. The paper also summarizes the main scientific questions that PEEX is going to tackle in the future.
K. Ruusuvuori, P. Hietala, O. Kupiainen-Määttä, T. Jokinen, H. Junninen, M. Sipilä, T. Kurtén, and H. Vehkamäki
Atmos. Meas. Tech., 8, 2577–2588, https://doi.org/10.5194/amt-8-2577-2015, https://doi.org/10.5194/amt-8-2577-2015, 2015
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Ionization reagents suitable for accurate measurements of the atmospheric gas-phase amine vapour concentrations are needed. Based on computational results, acetone is a viable option for use as an ionization reagent in CI-APi-TOF measurements on atmospheric dimethylamine. However, comparison between the computational and experimental results revealed notable discrepancies. Further study is still required before the acetone CI-APi-TOF can be considered a viable option in practice.
T. F. Mentel, M. Springer, M. Ehn, E. Kleist, I. Pullinen, T. Kurtén, M. Rissanen, A. Wahner, and J. Wildt
Atmos. Chem. Phys., 15, 6745–6765, https://doi.org/10.5194/acp-15-6745-2015, https://doi.org/10.5194/acp-15-6745-2015, 2015
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We studied a series of cycloalkenes and methyl-substituted alkenes in order to elucidate the structural pre-requisites and chemical pathways to the recently discovered class of highly oxidized molecules ELVOC (Ehn et al., Nature, 2014). ELVOC may totally change the view on (parts of) the mechanism of SOA formation. We present results which support recent observations of H shifts from C-H to peroxy radicals, highlighting the pivotal role of peroxyradicals in organic atmospheric chemistry.
N. T. Tsona, N. Bork, and H. Vehkamäki
Atmos. Chem. Phys., 15, 495–503, https://doi.org/10.5194/acp-15-495-2015, https://doi.org/10.5194/acp-15-495-2015, 2015
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
N. Bork, J. Elm, T. Olenius, and H. Vehkamäki
Atmos. Chem. Phys., 14, 12023–12030, https://doi.org/10.5194/acp-14-12023-2014, https://doi.org/10.5194/acp-14-12023-2014, 2014
I. K. Ortega, T. Olenius, O. Kupiainen-Määttä, V. Loukonen, T. Kurtén, and H. Vehkamäki
Atmos. Chem. Phys., 14, 7995–8007, https://doi.org/10.5194/acp-14-7995-2014, https://doi.org/10.5194/acp-14-7995-2014, 2014
K. Ruusuvuori, T. Kurtén, I. K. Ortega, J. Faust, and H. Vehkamäki
Atmos. Chem. Phys., 13, 10397–10404, https://doi.org/10.5194/acp-13-10397-2013, https://doi.org/10.5194/acp-13-10397-2013, 2013
N. Bork, T. Kurtén, and H. Vehkamäki
Atmos. Chem. Phys., 13, 3695–3703, https://doi.org/10.5194/acp-13-3695-2013, https://doi.org/10.5194/acp-13-3695-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Physics (physical properties and processes)
Revealing dominant patterns of aerosol regimes in the lower troposphere and their evolution from preindustrial times to the future in global climate model simulations
Improving estimation of a record-breaking east Asian dust storm emission with lagged aerosol Ångström exponent observations
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
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
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
Decomposing the effective radiative forcing of anthropogenic aerosols based on CMIP6 Earth system models
The role of interfacial tension in the size-dependent phase separation of atmospheric aerosol particles
Modeling impacts of dust mineralogy on fast climate response
Representation of iron aerosol size distributions is critical in evaluating atmospheric soluble iron input to the ocean
Gaps in our understanding of ice-nucleating particle sources exposed by global simulation of the UK climate model
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
Solar radiation estimation in West Africa: impact of dust conditions during 2021 dry season
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
Biomass Burning Emissions Analysis Based on MODIS AOD and AeroCom Multi-Model Simulations
Global aviation contrail climate effects from 2019 to 2021
Multi-model effective radiative forcing of the 2020 sulphur cap for shipping
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
Warming effects of reduced sulfur emissions from shipping
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
Tropospheric aerosols over the western North Atlantic Ocean during the winter and summer campaigns of ACTIVATE 2020: Life cycle, transport, and distribution
Simulated phase state and viscosity of secondary organic aerosols over China
Comparing the simulated influence of biomass burning plumes on low-level clouds over the southeastern Atlantic under varying smoke conditions
A global dust emission dataset for estimating dust radiative forcings in climate models
Improved simulations of biomass burning aerosol optical properties and lifetimes in the NASA GEOS Model during the ORACLES-I campaign
Sharp increase in Saharan dust intrusions over the western Euro-Mediterranean in February–March 2020–2022 and associated atmospheric circulation
Temporal and spatial variations in dust activity in Australia based on remote sensing and reanalysis datasets
Sensitivity of global direct aerosol shortwave radiative forcing to uncertainties in aerosol optical properties
Molecular-level study on the role of methanesulfonic acid in iodine oxoacid nucleation
Regional to global distributions, trends, and drivers of biogenic volatile organic compound emission from 2001 to 2020
Impacts of ice-nucleating particles on cirrus clouds and radiation derived from global model simulations with MADE3 in EMAC
Seasonal characteristics of emission, distribution, and radiative effect of marine organic aerosols over the western Pacific Ocean: an investigation with a coupled regional climate aerosol model
Fire–precipitation interactions amplify the quasi-biennial variability in fires over southern Mexico and Central America
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.
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.
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.
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.
Ryan Schmedding and Andreas Zuend
EGUsphere, https://doi.org/10.5194/egusphere-2024-1690, https://doi.org/10.5194/egusphere-2024-1690, 2024
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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.
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.
Mingxu Liu, Hitoshi Matsui, Douglas Hamilton, Sagar Rathod, Kara Lamb, and Natalie Mahowald
EGUsphere, https://doi.org/10.5194/egusphere-2024-1454, https://doi.org/10.5194/egusphere-2024-1454, 2024
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Atmospheric aerosol deposition provides iron to promote marine primary production, yet its amount remains highly uncertain. This study demonstrates that iron-containing particle size at emission is a critical factor in regulating their input to open oceans by performing global aerosol simulations. Further observational constraints on this are needed to reduce modelling uncertainties.
Ross J. Herbert, Alberto Sanchez-Marroquin, Daniel P. Grosvenor, Kirsty J. Pringle, Stephen R. Arnold, Benjamin J. Murray, and Kenneth S. Carslaw
EGUsphere, https://doi.org/10.5194/egusphere-2024-1538, https://doi.org/10.5194/egusphere-2024-1538, 2024
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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 aerosol that are known to nucleate ice. Here we report the first steps towards representing ice-nucleating particles within the UK's 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.
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.
Léo Clauzel, Sandrine Anquetin, Christophe Lavaysse, Gilles Bergametti, Christel Bouet, Guillaume Siour, Rémy Lapere, Béatrice Marticorena, and Jennie Thomas
EGUsphere, https://doi.org/10.5194/egusphere-2024-1604, https://doi.org/10.5194/egusphere-2024-1604, 2024
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Solar energy production in West Africa is set to rise, needing accurate solar radiation estimates, which is 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 cut 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.
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.
Mariya Petrenko, Ralph Kahn, Mian Chin, Susanne E. Bauer, Tommi Bergman, Huisheng Bian, Gabriele Curci, Ben Johnson, Johannes 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
EGUsphere, https://doi.org/10.5194/egusphere-2024-1487, https://doi.org/10.5194/egusphere-2024-1487, 2024
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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.
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.
Ragnhild Bieltvedt Skeie, Rachael Byrom, Øivind Hodnebrog, Caroline Jouan, and Gunnar Myhre
EGUsphere, https://doi.org/10.5194/egusphere-2024-1394, https://doi.org/10.5194/egusphere-2024-1394, 2024
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In 2020 new regulations by the International Maritime Organization of sulphur emissions came into force that reduced emissions of SO2 from the shipping sector by approximately 80 %. In this study, we use multiple models to calculate by how much the Earth energy balance changed due to the emission reduction, 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 two to three years.
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.
Masaru Yoshioka, Daniel P. Grosvenor, Ben B. B. Booth, Colin P. Morice, and Kenneth S. Carslaw
EGUsphere, https://doi.org/10.5194/egusphere-2024-1428, https://doi.org/10.5194/egusphere-2024-1428, 2024
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Sulfur emissions from shipping has been reduced by about 80 % as a result of the new regulation introduced in 2020. This has reduced aerosol in the atmosphere and its cooling effect through interactions with clouds. As a result, our coupled climate model simulations predict a global warming of 0.04 K averaged over three decades, potentially surpassing the Paris target of 1.5 K or contributing to recent temperature spikes, particularly notable in the Arctic with a mean warming of 0.15 K.
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.
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, Jason L. Tackett, Mark A. Vaughan, Yongxiang Hu, Glenn S. Diskin, John B. Nowak, Joshua P. DiGangi, Yonghoon Choi, Christoph A. Keller, and Matthew S. Johnson
EGUsphere, https://doi.org/10.5194/egusphere-2024-1127, https://doi.org/10.5194/egusphere-2024-1127, 2024
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We use the GEOS-Chem model to simulate aerosols over the western North Atlantic Ocean (WNAO) during the winter and summer campaigns of ACTIVATE 2020. Model results are evaluated against in situ and remote sensing measurements from two aircraft as well as ground-based and satellite observations. The improved understanding of the aerosol life cycle, composition, transport pathways, and distribution has important implications for characterizing aerosol-cloud-meteorology interactions over the WNAO.
Zhiqiang Zhang, Ying Li, Haiyan Ran, Junling An, Yu Qu, Wei Zhou, Weiqi Xu, Weiwei Hu, Hongbin Xie, Zifa Wang, Yele Sun, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 4809–4826, https://doi.org/10.5194/acp-24-4809-2024, https://doi.org/10.5194/acp-24-4809-2024, 2024
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Secondary organic aerosols (SOAs) can exist in liquid, semi-solid, or amorphous solid states, which are rarely accounted for in current chemical transport models. We predict the phase state of SOA particles over China and find that in northwestern China SOA particles are mostly highly viscous or glassy solid. Our results indicate that the particle phase state should be considered in SOA formation in chemical transport models for more accurate prediction of SOA mass concentrations.
Alejandro Baró Pérez, Michael S. Diamond, Frida A.-M. Bender, Abhay Devasthale, Matthias Schwarz, Julien Savre, Juha Tonttila, Harri Kokkola, Hyunho Lee, David Painemal, and Annica M. L. Ekman
Atmos. Chem. Phys., 24, 4591–4610, https://doi.org/10.5194/acp-24-4591-2024, https://doi.org/10.5194/acp-24-4591-2024, 2024
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We use a numerical model to study interactions between humid light-absorbing aerosol plumes, clouds, and radiation over the southeast Atlantic. We find that the warming produced by the aerosols reduces cloud cover, especially in highly polluted situations. Aerosol impacts on drizzle play a minor role. However, aerosol effects on cloud reflectivity and moisture-induced changes in cloud cover dominate the climatic response and lead to an overall cooling by the biomass burning plumes.
Danny M. Leung, Jasper F. Kok, Longlei Li, David M. Lawrence, Natalie M. Mahowald, Simone Tilmes, and Erik Kluzek
EGUsphere, https://doi.org/10.5194/egusphere-2024-1124, https://doi.org/10.5194/egusphere-2024-1124, 2024
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This study derives a desert dust emission dataset for 1841–2000, by employing a combination of observed dust records from sedimentary cores as well as 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 match better against observations than other mechanistic models.
Sampa Das, Peter R. Colarco, Huisheng Bian, and Santiago Gassó
Atmos. Chem. Phys., 24, 4421–4449, https://doi.org/10.5194/acp-24-4421-2024, https://doi.org/10.5194/acp-24-4421-2024, 2024
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The smoke aerosols emitted from vegetation burning can alter the regional energy budget via multiple pathways. We utilized detailed observations from the NASA ORACLES airborne campaign based in Namibia during September 2016 to improve the representation of smoke aerosol properties and lifetimes in our GEOS Earth system model. The improved model simulations are for the first time able to capture the observed changes in the smoke absorption during long-range plume transport.
Emilio Cuevas-Agulló, David Barriopedro, Rosa Delia García, Silvia Alonso-Pérez, Juan Jesús González-Alemán, Ernest Werner, David Suárez, Juan José Bustos, Gerardo García-Castrillo, Omaira García, África Barreto, and Sara Basart
Atmos. Chem. Phys., 24, 4083–4104, https://doi.org/10.5194/acp-24-4083-2024, https://doi.org/10.5194/acp-24-4083-2024, 2024
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During February–March (FM) 2020–2022, unusually intense dust storms from northern Africa hit the western Euro-Mediterranean (WEM). Using dust products from satellites and atmospheric reanalysis for 2003–2022, results show that cut-off lows and European blocking are key drivers of FM dust intrusions over the WEM. A higher frequency of cut-off lows associated with subtropical ridges is observed in the late 2020–2022 period.
Yahui Che, Bofu Yu, and Katherine Bracco
Atmos. Chem. Phys., 24, 4105–4128, https://doi.org/10.5194/acp-24-4105-2024, https://doi.org/10.5194/acp-24-4105-2024, 2024
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Dust events occur more frequently during the Austral spring and summer in dust regions, including central Australia, the southwest of Western Australia, and the northern and southern regions of eastern Australia using remote sensing and reanalysis datasets. High-concentration dust is distributed around central Australia and in the downwind northern and southern Australia. Typically, around 50 % of the dust lifted settles on Australian land, with the remaining half being deposited in the ocean.
Jonathan Elsey, Nicolas Bellouin, and Claire Ryder
Atmos. Chem. Phys., 24, 4065–4081, https://doi.org/10.5194/acp-24-4065-2024, https://doi.org/10.5194/acp-24-4065-2024, 2024
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Aerosols influence the Earth's energy balance. The uncertainty in this radiative forcing is large depending partly on uncertainty in measurements of aerosol optical properties. We have developed a freely available new framework of millions of radiative transfer simulations spanning aerosol uncertainty and assess the impact on radiative forcing uncertainty. We find that reducing these uncertainties would reduce radiative forcing uncertainty, but non-aerosol uncertainties must also be considered.
Jing Li, Nan Wu, Biwu Chu, An Ning, and Xiuhui Zhang
Atmos. Chem. Phys., 24, 3989–4000, https://doi.org/10.5194/acp-24-3989-2024, https://doi.org/10.5194/acp-24-3989-2024, 2024
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Iodic acid (HIO3) nucleates with iodous acid (HIO2) efficiently in marine areas; however, whether methanesulfonic acid (MSA) can synergistically participate in the HIO3–HIO2-based nucleation is unclear. We provide molecular-level evidence that MSA can efficiently promote the formation of HIO3–HIO2-based clusters using a theoretical approach. The proposed MSA-enhanced iodine nucleation mechanism may help us to deeply understand marine new particle formation events with bursts of iodine particles.
Hao Wang, Xiaohong Liu, Chenglai Wu, and Guangxing Lin
Atmos. Chem. Phys., 24, 3309–3328, https://doi.org/10.5194/acp-24-3309-2024, https://doi.org/10.5194/acp-24-3309-2024, 2024
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We quantified different global- and regional-scale drivers of biogenic volatile organic compound (BVOC) emission trends over the past 20 years. The results show that global greening trends significantly boost BVOC emissions and deforestation reduces BVOC emissions in South America and Southeast Asia. Elevated temperature in Europe and increased soil moisture in East and South Asia enhance BVOC emissions. The results deepen our understanding of long-term BVOC emission trends in hotspots.
Christof G. Beer, Johannes Hendricks, and Mattia Righi
Atmos. Chem. Phys., 24, 3217–3240, https://doi.org/10.5194/acp-24-3217-2024, https://doi.org/10.5194/acp-24-3217-2024, 2024
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Ice-nucleating particles (INPs) have important influences on cirrus clouds and the climate system; however, the understanding of their global impacts is still uncertain. We perform numerical simulations with a global aerosol–climate model to analyse INP-induced cirrus changes and the resulting climate impacts. We evaluate various sources of uncertainties, e.g. the ice-nucleating ability of INPs and the role of model dynamics, and provide a new estimate for the global INP–cirrus effect.
Jiawei Li, Zhiwei Han, Pingqing Fu, Xiaohong Yao, and Mingjie Liang
Atmos. Chem. Phys., 24, 3129–3161, https://doi.org/10.5194/acp-24-3129-2024, https://doi.org/10.5194/acp-24-3129-2024, 2024
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Organic aerosols of marine origin are important for aerosol climatic effects but are poorly understood. For the first time, an online coupled regional chemistry–climate model is applied to explore the characteristics of emission, distribution, and direct and indirect radiative effects of marine organic aerosols over the western Pacific, which reveals an important role of marine organic aerosols in perturbing cloud and radiation and promotes understanding of global aerosol climatic impact.
Yawen Liu, Yun Qian, Philip J. Rasch, Kai Zhang, Lai-yung Ruby Leung, Yuhang Wang, Minghuai Wang, Hailong Wang, Xin Huang, and Xiu-Qun Yang
Atmos. Chem. Phys., 24, 3115–3128, https://doi.org/10.5194/acp-24-3115-2024, https://doi.org/10.5194/acp-24-3115-2024, 2024
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Fire management has long been a challenge. Here we report that spring-peak fire activity over southern Mexico and Central America (SMCA) has a distinct quasi-biennial signal by measuring multiple fire metrics. This signal is initially driven by quasi-biennial variability in precipitation and is further amplified by positive feedback of fire–precipitation interaction at short timescales. This work highlights the importance of fire–climate interactions in shaping fires on an interannual scale.
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The rate of collisions between molecules or clusters is used to determine particle formation in the atmosphere. The basic approach is to treat the colliding particles as noninteracting hard spheres. By using atomistic simulations with a realistic force field and theoretical approaches, we showed that the actual collision rate of two sulfuric acid molecules is more than twice as high as that for hard spheres. The results of this study will improve models of atmospheric particle growth.
The rate of collisions between molecules or clusters is used to determine particle formation in...
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