Articles | Volume 25, issue 18
https://doi.org/10.5194/acp-25-11317-2025
© Author(s) 2025. 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-25-11317-2025
© Author(s) 2025. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
25 Sep 2025
Research article |
| 25 Sep 2025
| 25 Sep 2025
Homogeneous ice nucleation in adsorbed water films: a theoretical approach
Finnish Meteorological Institute, 00101 Helsinki, Finland
Department of Technical Physics, University of Eastern Finland, 70211 Kuopio, Finland
Golnaz Roudsari
Finnish Meteorological Institute, 00101 Helsinki, Finland
Ana A. Piedehierro
Finnish Meteorological Institute, 00101 Helsinki, Finland
André Welti
Finnish Meteorological Institute, 00101 Helsinki, Finland
Related authors
Aino Ovaska, Elio Rauth, Daniel Holmberg, Paulo Artaxo, John Backman, Benjamin Bergmans, Don Collins, Marco Aurélio Franco, Shahzad Gani, Roy M. Harrison, Rakes K. Hooda, Tareq Hussein, Antti-Pekka Hyvärinen, Kerneels Jaars, Adam Kristensson, Markku Kulmala, Lauri Laakso, Ari Laaksonen, Nikolaos Mihalopoulos, Colin O'Dowd, Jakub Ondracek, Tuukka Petäjä, Kristina Plauškaitė, Mira Pöhlker, Ximeng Qi, Peter Tunved, Ville Vakkari, Alfred Wiedensohler, Kai Puolamäki, Tuomo Nieminen, Veli-Matti Kerminen, Victoria A. Sinclair, and Pauli Paasonen
Aerosol Research Discuss., https://doi.org/10.5194/ar-2025-18, https://doi.org/10.5194/ar-2025-18, 2025
Preprint under review for AR
Short summary
Short summary
We trained machine learning models to estimate the number of aerosol particles large enough to form clouds and generated daily estimates for the entire globe. The models performed well in many continental regions but struggled in remote and marine areas. Still, this approach offers a way to quantify these particles in areas that lack direct measurements, helping us understand their influence on clouds and climate on a global scale.
Kasper Juurikkala, Christina J. Williamson, Karl D. Froyd, Jonathan Dean-Day, and Ari Laaksonen
EGUsphere, https://doi.org/10.5194/egusphere-2025-163, https://doi.org/10.5194/egusphere-2025-163, 2025
Short summary
Short summary
This study uses UCLALES-SALSA simulations to investigate synoptic cirrus clouds from NASA’s MACPEX campaign. Results show that prior heterogeneous ice nucleation depletes ice nuclei, creating conditions for subsequent homogeneous freezing. The findings highlight limitations of ice residual analysis in capturing cirrus evolution and provide insights into aerosol-cloud interactions critical to atmospheric and climate processes.
Ari Laaksonen
Aerosol Research, 2, 343–351, https://doi.org/10.5194/ar-2-343-2024, https://doi.org/10.5194/ar-2-343-2024, 2024
Short summary
Short summary
Insoluble aerosol particles such as minerals and black carbon can trigger freezing inside clouds, which leads to rain formation. However, both particle types are relatively poor nuclei for cloud droplets. In this work, theoretical calculations are presented about the ability of surface-tension-reducing compounds to promote cloud drop formation around insoluble aerosols. The calculations indicate that such surfactants can be efficient in “smuggling” insoluble particles into cloud droplets.
Mária Lbadaoui-Darvas, Ari Laaksonen, and Athanasios Nenes
Atmos. Chem. Phys., 23, 10057–10074, https://doi.org/10.5194/acp-23-10057-2023, https://doi.org/10.5194/acp-23-10057-2023, 2023
Short summary
Short summary
Heterogeneous ice nucleation is the main ice formation mechanism in clouds. The mechanism of different freezing modes is to date unknown, which results in large model biases. Experiments do not allow for direct observation of ice nucleation at its native resolution. This work uses first principles molecular simulations to determine the mechanism of the least-understood ice nucleation mode and link it to adsorption through a novel modeling framework that unites ice and droplet formation.
Kimmo Korhonen, Thomas Bjerring Kristensen, John Falk, Vilhelm B. Malmborg, Axel Eriksson, Louise Gren, Maja Novakovic, Sam Shamun, Panu Karjalainen, Lassi Markkula, Joakim Pagels, Birgitta Svenningsson, Martin Tunér, Mika Komppula, Ari Laaksonen, and Annele Virtanen
Atmos. Chem. Phys., 22, 1615–1631, https://doi.org/10.5194/acp-22-1615-2022, https://doi.org/10.5194/acp-22-1615-2022, 2022
Short summary
Short summary
We investigated the ice-nucleating abilities of particulate emissions from a modern diesel engine using the portable ice-nuclei counter SPIN, a continuous-flow diffusion chamber instrument. Three different fuels were studied without blending, including fossil diesel and two renewable fuels, testing different emission aftertreatment systems and photochemical aging. We found that the diesel emissions were inefficient ice nuclei, and aging had no or little effect on their ice-nucleating abilities.
Ana A. Piedehierro, André Welti, Angela Buchholz, Kimmo Korhonen, Iida Pullinen, Ilkka Summanen, Annele Virtanen, and Ari Laaksonen
Atmos. Chem. Phys., 21, 11069–11078, https://doi.org/10.5194/acp-21-11069-2021, https://doi.org/10.5194/acp-21-11069-2021, 2021
Short summary
Short summary
Ice crystals in cirrus clouds contain particles that start ice formation. We study whether particles forming above boreal forests can help in the making of cirrus clouds and if the water content in the particles affects this property. In the laboratory, we made boreal-forest-like particles and cooled and humidified them to measure whether an ice crystal develops. We found that only when dry can these particles form an ice crystal but no better than solution droplets.
André Welti, Kimmo Korhonen, Pasi Miettinen, Ana A. Piedehierro, Yrjö Viisanen, Annele Virtanen, and Ari Laaksonen
Atmos. Meas. Tech., 13, 7059–7067, https://doi.org/10.5194/amt-13-7059-2020, https://doi.org/10.5194/amt-13-7059-2020, 2020
Short summary
Short summary
We describe a modification of the SPectrometer for Ice Nuclei (SPIN) chamber to study ice nucleation at low temperatures, relevant for ice formation in cirrus clouds. Validation experiments of homogeneous freezing of aqueous ammonium sulfate droplets and heterogeneous ice nucleation on silver iodide particles are included to demonstrate the advantages of the modified SPIN chamber for the investigation of ice nucleation in the extended temperature range.
Ari Laaksonen, Jussi Malila, and Athanasios Nenes
Atmos. Chem. Phys., 20, 13579–13589, https://doi.org/10.5194/acp-20-13579-2020, https://doi.org/10.5194/acp-20-13579-2020, 2020
Short summary
Short summary
Aerosol particles containing black carbon are ubiquitous in the atmosphere and originate from combustion processes. We examine their capability to act as condensation centers for water vapor. We make use of published experimental data sets for different types of black carbon particles, ranging from very pure particles to particles that contain both black carbon and water soluble organic matter, and we show that a recently developed theory reproduces most of the experimental results.
Aino Ovaska, Elio Rauth, Daniel Holmberg, Paulo Artaxo, John Backman, Benjamin Bergmans, Don Collins, Marco Aurélio Franco, Shahzad Gani, Roy M. Harrison, Rakes K. Hooda, Tareq Hussein, Antti-Pekka Hyvärinen, Kerneels Jaars, Adam Kristensson, Markku Kulmala, Lauri Laakso, Ari Laaksonen, Nikolaos Mihalopoulos, Colin O'Dowd, Jakub Ondracek, Tuukka Petäjä, Kristina Plauškaitė, Mira Pöhlker, Ximeng Qi, Peter Tunved, Ville Vakkari, Alfred Wiedensohler, Kai Puolamäki, Tuomo Nieminen, Veli-Matti Kerminen, Victoria A. Sinclair, and Pauli Paasonen
Aerosol Research Discuss., https://doi.org/10.5194/ar-2025-18, https://doi.org/10.5194/ar-2025-18, 2025
Preprint under review for AR
Short summary
Short summary
We trained machine learning models to estimate the number of aerosol particles large enough to form clouds and generated daily estimates for the entire globe. The models performed well in many continental regions but struggled in remote and marine areas. Still, this approach offers a way to quantify these particles in areas that lack direct measurements, helping us understand their influence on clouds and climate on a global scale.
Guangyu Li, André Welti, Iris Thurnherr, Ulrike Lohmann, and Zamin A. Kanji
EGUsphere, https://doi.org/10.5194/egusphere-2025-2798, https://doi.org/10.5194/egusphere-2025-2798, 2025
Short summary
Short summary
This study presents ship-based measurements of summertime ice-nucleating particles (INPs) over the data-scarce Eurasian-Arctic Seas. We found that INPs are driven by both local and regional sources, with the highest levels observed near land and over ice-free waters. This study is highlighted for improving the understanding of INP abundance, sources, and their role in cloud processes in the rapidly warming Arctic.
Kasper Juurikkala, Christina J. Williamson, Karl D. Froyd, Jonathan Dean-Day, and Ari Laaksonen
EGUsphere, https://doi.org/10.5194/egusphere-2025-163, https://doi.org/10.5194/egusphere-2025-163, 2025
Short summary
Short summary
This study uses UCLALES-SALSA simulations to investigate synoptic cirrus clouds from NASA’s MACPEX campaign. Results show that prior heterogeneous ice nucleation depletes ice nuclei, creating conditions for subsequent homogeneous freezing. The findings highlight limitations of ice residual analysis in capturing cirrus evolution and provide insights into aerosol-cloud interactions critical to atmospheric and climate processes.
Olivia G. Norman, Colette L. Heald, Solomon Bililign, Pedro Campuzano-Jost, Hugh Coe, Marc N. Fiddler, Jaime R. Green, Jose L. Jimenez, Katharina Kaiser, Jin Liao, Ann M. Middlebrook, Benjamin A. Nault, John B. Nowak, Johannes Schneider, and André Welti
Atmos. Chem. Phys., 25, 771–795, https://doi.org/10.5194/acp-25-771-2025, https://doi.org/10.5194/acp-25-771-2025, 2025
Short summary
Short summary
This study finds that one component of secondary inorganic aerosols, nitrate, is greatly overestimated by a global atmospheric chemistry model compared to observations from 11 flight campaigns. None of the loss and production pathways explored can explain the nitrate bias alone. The model’s inability to capture the variability in the observations remains and requires future investigation to avoid biases in policy-related studies (i.e., air quality, health, climate impacts of these aerosols).
Ari Laaksonen
Aerosol Research, 2, 343–351, https://doi.org/10.5194/ar-2-343-2024, https://doi.org/10.5194/ar-2-343-2024, 2024
Short summary
Short summary
Insoluble aerosol particles such as minerals and black carbon can trigger freezing inside clouds, which leads to rain formation. However, both particle types are relatively poor nuclei for cloud droplets. In this work, theoretical calculations are presented about the ability of surface-tension-reducing compounds to promote cloud drop formation around insoluble aerosols. The calculations indicate that such surfactants can be efficient in “smuggling” insoluble particles into cloud droplets.
Hannah C. Frostenberg, André Welti, Mikael Luhr, Julien Savre, Erik S. Thomson, and Luisa Ickes
Atmos. Chem. Phys., 23, 10883–10900, https://doi.org/10.5194/acp-23-10883-2023, https://doi.org/10.5194/acp-23-10883-2023, 2023
Short summary
Short summary
Observations show that ice-nucleating particle concentrations (INPCs) have a large variety and follow lognormal distributions for a given temperature. We introduce a new immersion freezing parameterization that applies this lognormal behavior. INPCs are drawn randomly from a temperature-dependent lognormal distribution. We then show that the ice content of the modeled Arctic stratocumulus cloud is highly sensitive to the probability of drawing large INPCs.
Mária Lbadaoui-Darvas, Ari Laaksonen, and Athanasios Nenes
Atmos. Chem. Phys., 23, 10057–10074, https://doi.org/10.5194/acp-23-10057-2023, https://doi.org/10.5194/acp-23-10057-2023, 2023
Short summary
Short summary
Heterogeneous ice nucleation is the main ice formation mechanism in clouds. The mechanism of different freezing modes is to date unknown, which results in large model biases. Experiments do not allow for direct observation of ice nucleation at its native resolution. This work uses first principles molecular simulations to determine the mechanism of the least-understood ice nucleation mode and link it to adsorption through a novel modeling framework that unites ice and droplet formation.
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
Short summary
Short summary
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
Short summary
Short summary
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.
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
Short summary
Short summary
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.
Christian Tatzelt, Silvia Henning, André Welti, Andrea Baccarini, Markus Hartmann, Martin Gysel-Beer, Manuela van Pinxteren, Robin L. Modini, Julia Schmale, and Frank Stratmann
Atmos. Chem. Phys., 22, 9721–9745, https://doi.org/10.5194/acp-22-9721-2022, https://doi.org/10.5194/acp-22-9721-2022, 2022
Short summary
Short summary
We present the abundance and origin of cloud-relevant aerosol particles in the preindustral-like conditions of the Southern Ocean (SO) during austral summer. Cloud condensation nuclei (CCN) and ice-nucleating particles (INP) were measured during a circum-Antarctic scientific cruise with in situ instrumentation and offline filter measurements, respectively. Transport processes were found to play an equally important role as local sources for both the CCN and INP population of the SO.
Kimmo Korhonen, Thomas Bjerring Kristensen, John Falk, Vilhelm B. Malmborg, Axel Eriksson, Louise Gren, Maja Novakovic, Sam Shamun, Panu Karjalainen, Lassi Markkula, Joakim Pagels, Birgitta Svenningsson, Martin Tunér, Mika Komppula, Ari Laaksonen, and Annele Virtanen
Atmos. Chem. Phys., 22, 1615–1631, https://doi.org/10.5194/acp-22-1615-2022, https://doi.org/10.5194/acp-22-1615-2022, 2022
Short summary
Short summary
We investigated the ice-nucleating abilities of particulate emissions from a modern diesel engine using the portable ice-nuclei counter SPIN, a continuous-flow diffusion chamber instrument. Three different fuels were studied without blending, including fossil diesel and two renewable fuels, testing different emission aftertreatment systems and photochemical aging. We found that the diesel emissions were inefficient ice nuclei, and aging had no or little effect on their ice-nucleating abilities.
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
Short summary
Short summary
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.
Markus Hartmann, Xianda Gong, Simonas Kecorius, Manuela van Pinxteren, Teresa Vogl, André Welti, Heike Wex, Sebastian Zeppenfeld, Hartmut Herrmann, Alfred Wiedensohler, and Frank Stratmann
Atmos. Chem. Phys., 21, 11613–11636, https://doi.org/10.5194/acp-21-11613-2021, https://doi.org/10.5194/acp-21-11613-2021, 2021
Short summary
Short summary
Ice-nucleating particles (INPs) are not well characterized in the Arctic despite their importance for the Arctic energy budget. Little is known about their nature (mineral or biological) and sources (terrestrial or marine, long-range transport or local). We find indications that, at the beginning of the melt season, a local, biogenic, probably marine source is likely, but significant enrichment of INPs has to take place from the ocean to the aerosol phase.
Ana A. Piedehierro, André Welti, Angela Buchholz, Kimmo Korhonen, Iida Pullinen, Ilkka Summanen, Annele Virtanen, and Ari Laaksonen
Atmos. Chem. Phys., 21, 11069–11078, https://doi.org/10.5194/acp-21-11069-2021, https://doi.org/10.5194/acp-21-11069-2021, 2021
Short summary
Short summary
Ice crystals in cirrus clouds contain particles that start ice formation. We study whether particles forming above boreal forests can help in the making of cirrus clouds and if the water content in the particles affects this property. In the laboratory, we made boreal-forest-like particles and cooled and humidified them to measure whether an ice crystal develops. We found that only when dry can these particles form an ice crystal but no better than solution droplets.
André Welti, Kimmo Korhonen, Pasi Miettinen, Ana A. Piedehierro, Yrjö Viisanen, Annele Virtanen, and Ari Laaksonen
Atmos. Meas. Tech., 13, 7059–7067, https://doi.org/10.5194/amt-13-7059-2020, https://doi.org/10.5194/amt-13-7059-2020, 2020
Short summary
Short summary
We describe a modification of the SPectrometer for Ice Nuclei (SPIN) chamber to study ice nucleation at low temperatures, relevant for ice formation in cirrus clouds. Validation experiments of homogeneous freezing of aqueous ammonium sulfate droplets and heterogeneous ice nucleation on silver iodide particles are included to demonstrate the advantages of the modified SPIN chamber for the investigation of ice nucleation in the extended temperature range.
André Welti, E. Keith Bigg, Paul J. DeMott, Xianda Gong, Markus Hartmann, Mike Harvey, Silvia Henning, Paul Herenz, Thomas C. J. Hill, Blake Hornblow, Caroline Leck, Mareike Löffler, Christina S. McCluskey, Anne Marie Rauker, Julia Schmale, Christian Tatzelt, Manuela van Pinxteren, and Frank Stratmann
Atmos. Chem. Phys., 20, 15191–15206, https://doi.org/10.5194/acp-20-15191-2020, https://doi.org/10.5194/acp-20-15191-2020, 2020
Short summary
Short summary
Ship-based measurements of maritime ice nuclei concentrations encompassing all oceans are compiled. From this overview it is found that maritime ice nuclei concentrations are typically 10–100 times lower than over continents, while concentrations are surprisingly similar in different oceanic regions. The analysis of the influence of ship emissions shows no effect on the data, making ship-based measurements an efficient strategy for the large-scale exploration of ice nuclei concentrations.
Ari Laaksonen, Jussi Malila, and Athanasios Nenes
Atmos. Chem. Phys., 20, 13579–13589, https://doi.org/10.5194/acp-20-13579-2020, https://doi.org/10.5194/acp-20-13579-2020, 2020
Short summary
Short summary
Aerosol particles containing black carbon are ubiquitous in the atmosphere and originate from combustion processes. We examine their capability to act as condensation centers for water vapor. We make use of published experimental data sets for different types of black carbon particles, ranging from very pure particles to particles that contain both black carbon and water soluble organic matter, and we show that a recently developed theory reproduces most of the experimental results.
Hans-Christian Clemen, Johannes Schneider, Thomas Klimach, Frank Helleis, Franziska Köllner, Andreas Hünig, Florian Rubach, Stephan Mertes, Heike Wex, Frank Stratmann, André Welti, Rebecca Kohl, Fabian Frank, and Stephan Borrmann
Atmos. Meas. Tech., 13, 5923–5953, https://doi.org/10.5194/amt-13-5923-2020, https://doi.org/10.5194/amt-13-5923-2020, 2020
Short summary
Short summary
We improved the efficiency of a single-particle mass spectrometer with a newly developed aerodynamic lens system, delayed ion extraction, and better electric shielding. The new components result in significantly improved particle analysis and sample statistics. This is particularly important for measurements of low-number-density particles, such as ice-nucleating particles, and for aircraft-based measurements at high altitudes or where high temporal and spatial resolution is required.
Aikaterini Bougiatioti, Athanasios Nenes, Jack J. Lin, Charles A. Brock, Joost A. de Gouw, Jin Liao, Ann M. Middlebrook, and André Welti
Atmos. Chem. Phys., 20, 12163–12176, https://doi.org/10.5194/acp-20-12163-2020, https://doi.org/10.5194/acp-20-12163-2020, 2020
Short summary
Short summary
The number concentration of droplets in clouds in the summertime in the southeastern United States is influenced by aerosol variations but limited by the strong competition for supersaturated water vapor. Concurrent variations in vertical velocity magnify the response of cloud droplet number to aerosol increases by up to a factor of 5. Omitting the covariance of vertical velocity with aerosol number may therefore bias estimates of the cloud albedo effect from aerosols.
Cited articles
Barahona, D.: On the thermodynamic and kinetic aspects of immersion ice nucleation, Atmos. Chem. Phys., 18, 17119–17141, https://doi.org/10.5194/acp-18-17119-2018, 2018. a
Boinovich, L. B. and Emelyanenko, A. M.: Experimental determination of the surface energy of polycrystalline ice, Doklady Phys. Chem., 459, 702–706, https://doi.org/10.1134/S0012501614120045, 2014. a
Chernoff, D. I. and Bertram, A. K.: Effects of sulfate coatings on the ice nucleation properties of a biological ice nucleus and several types of minerals, J. Geophys. Res., 115, D20205, https://doi.org/10.1029/2010JD014254, 2010. a
David, R. O., Marcolli, C., Fahrni, J., Qiu, Y., Perez Sirkin, Y. A., Molinero, V., Mahrt, F., Brühwiler, D., Lohmann, U., and Kanji, Z. A.: Pore condensation and freezing is responsible for ice formation below water saturation for porous particles, P. Natl. Acad. Sci. USA, 116, 8184–8189, https://doi.org/10.1073/pnas.1813647116, 2019. a, b, c, d
Eastwood, M. L., Cremel, S., Gehrke, C., Girard, E., and Bertram, A. K.: Ice nucleation on mineral dust particles: Onset conditions, nucleation rates and contact angles, J. Geophys. Res., 113, D22203, https://doi.org/10.1029/2008JD010639, 2008. a
Fletcher, N. H.: On ice-crystal production by aerosol particles, J. Atmos. Sci., 16, 173–180, https://doi.org/10.1175/1520-0469(1959)016<0173:OICPBA>2.0.CO;2, 1959. a
Fortes, A. D.: Accurate and precise lattice parameters of H2O and D2O ice Ih between 1.6 and 270K from high-resolution time-of-flight neutron powder diffraction data, Acta Crystallogr. B, 74, 196–216, https://doi.org/10.1107/S2052520618002159, 2018. a
Frenkel, J.: Kinetic Theory of Liquids, Oxford University Press, London, 1946. a
Haji-Akbari, A. and Debenedetti, P. G.: Computational investigation of surface freezing in a molecular model of water, P. Natl. Acad. Sci. USA, 114, 3316–3321, https://doi.org/10.1073/pnas.1620999114, 2017. a
Haji-Akbari, A. DeFever, R. S., Sarupia, S., and Debenedetti, P. G.: Suppression of sub-surface freezing in free-standing thin films of a coarse-grained model of water, Phys. Chem. Chem. Phys., 16, 25916–25927, https://doi.org/10.1039/C4CP03948C, 2014. a
Hale, B. N. and Plummer, P. L. M.: Molecular model for ice clusters in a supersaturated vapor, J. Chem. Phys., 61, 4012–4019, 1974. a
Halsey, G.: Physical Adsorption on Non‐Uniform Surfaces, J. Chem. Phys., 16, 931–937, https://doi.org/10.1063/1.1746689, 1948. a, b, c
Hayton, J. A., Davies, M. P., Whale, T. F., Michaelides, A., and Cox, S. J.: The limit of macroscopic homogeneous ice nucleation at the nanoscale, Faraday Discuss., 249, 210–218, https://doi.org/10.1039/d3fd00099k, 2024. a, b
Hill, T. L.: Theory of Physical Adsorption, Adv. Catal., 4, 211–258, https://doi.org/10.1016/S0360-0564(08)60615-X, 1952. a, b, c, d
Hrubý, J., Vinš, V., Mareš, R., and Kalová, J.: Surface tension of supercooled water: no inflection point down to −25 °C, J. Phys. Chem. Lett., 5, 425–428, https://doi.org/10.1021/jz402571a, 2014. a
Hyland, R. W. and Wexler, A.: Formulations for the thermodynamic properties of the saturated phases of H2O from 173.15 to 473.15 K, Ashrae Tran., 89, 500–520, 1983. a
Ibrahim, S., Romanias, M. N., Alleman, L. Y., Zeineddine, M. N., Angeli, G. K., Trikalitis, P. N., and Thevenet, F.: Water Interaction with Mineral Dust Aerosol: Particle Size and Hygroscopic Properties of Dust, ACS Earth Space Chem., 2, 376–386, https://doi.org/10.1021/acsearthspacechem.7b00152, 2018. a
Kalova, J.: Vapor Pressure of Supercooled Water, Int. J. Thermophys., 43, 165, https://doi.org/10.1007/s10765-022-03095-w, 2022. a
Kanagy, J. R.: Influence of temperature on the adsorption of water vapor by collagen and leather, J. Res. NBS, 44, 31–45, https://doi.org/10.6028/jres.044.004, 1950. a
Kanji, Z. A., Florea, O., and Abbatt, J. P. D.: Ice formation via deposition nucleation on mineral dust and organics: dependence of onset relative humidity on total particulate surface area, Environ. Res. Lett., 3, 025004, https://doi.org/10.1088/1748-9326/3/2/025004, 2008. a
Kulmala, M.: Nucleation as an aerosol physical problem, PhD thesis, University of Helsinki, ISBN 951-45-4678-4, 1988. a
Kumar, P., Sokolik, I. N., and Nenes, A.: Measurements of cloud condensation nuclei activity and droplet activation kinetics of fresh unprocessed regional dust samples and minerals, Atmos. Chem. Phys., 11, 3527–3541, https://doi.org/10.5194/acp-11-3527-2011, 2011. a, b, c, d
Laaksonen, A.: A Unifying Model for Adsorption and Nucleation of Vapors on Solid Surfaces, J. Phys. Chem. A, 119, 3736–3745, https://doi.org/10.1021/acs.jpca.5b00325, 2015. a
Laaksonen, A. and Malila, J.: Nucleation of water, Elsevier, Amsterdam, https://doi.org/10.1016/B978-0-12-814321-6.00012-9, 2021. a, b
Laaksonen, A., Malila, J., and Nenes, A.: Heterogeneous nucleation of water vapor on different types of black carbon particles, Atmos. Chem. Phys., 20, 13579–13589, https://doi.org/10.5194/acp-20-13579-2020, 2020. a
Laaksonen, A., Roudsari, G., Piedehierro, A. A., and Welti, A.: Homogeneous ice nucleation in adsorbed water films: A theoretical approach, Zenodo [code], https://doi.org/10.5281/zenodo.17087068, 2025a.
Laaksonen, A., Roudsari, G., Piedehierro, A. A., and Welti, A.: Model Code and Experimental Data Supporting “Homogeneous ice nucleation in adsorbed water films: A theoretical approach” by Laaksonen et al., Finnish Meteorological Institute [data set], https://doi.org/10.57707/FMI-B2SHARE.DE4F05CE04A344B284AE919A7665606A, 2025b.
Lbadaoui-Darvas, M., Laaksonen, A., and Nenes, A.: Deposition freezing, pore condensation freezing and adsorption: three processes, one description?, Atmos. Chem. Phys., 23, 10057–10074, https://doi.org/10.5194/acp-23-10057-2023, 2023. a, b
Leist, U., Ranke, W., and Al-Shamery, K.: Water adsorption and growth of ice on epitaxial Fe3O4(111), FeO(111) and Fe2O3(biphase), Phys. Chem. Chem. Phys., 5, 2435–2441, https://doi.org/10.1039/B212163H, 2003. a
Lü, Y., Zhang, X., and Chen, M.: Size effect on nucleation rate for homogeneous crystallization of nanoscale water film, J. Phys. Chem. B, 117, 10241–10249, https://doi.org/10.1021/jp404403k, 2013. a
Marcolli, C.: Deposition nucleation viewed as homogeneous or immersion freezing in pores and cavities, Atmos. Chem. Phys., 14, 2071–2104, https://doi.org/10.5194/acp-14-2071-2014, 2014. a
Marcolli, C.: Pre-activation of aerosol particles by ice preserved in pores, Atmos. Chem. Phys., 17, 1595–1622, https://doi.org/10.5194/acp-17-1595-2017, 2017. a
Marcolli, C.: Technical note: Fundamental aspects of ice nucleation via pore condensation and freezing including Laplace pressure and growth into macroscopic ice, Atmos. Chem. Phys., 20, 3209–3230, https://doi.org/10.5194/acp-20-3209-2020, 2020. a, b
McCafferty, E. and Zettlemoyer, A. C.: Adsorption of water vapour on α-Fe2O3, Discuss. Faraday Soc., 52, 239–254, https://doi.org/10.1039/DF9715200239, 1971. a
McClellan, A. L. and Harnsberger, H. F.: Cross-sectional areas of molecules adsorbed on solid surfaces, J. Colloid Interface Sci., 23, 577–599, https://doi.org/10.1016/0021-9797(67)90204-4, 1967. a
Nĕmec, T.: Estimation of ice-water interfacial energy based on pressure-dependent formulation of classical nucleation theory, Chem. Phys. Lett., 583, 64–68, https://doi.org/10.1016/j.cplett.2013.07.085, 2013. a
Pashley, R. and Kitchener, J.: Surface forces in adsorbed multilayers of water on quartz, J. Colloid Interface Sci., 71, 491–500, https://doi.org/10.1016/0021-9797(79)90323-0, 1979. a
Poling, B. E., Prausnitz, J. M., and O'Connell, J. P.: The Properties of Gases and Liquids, McGraw-Hill, New York, ISBN 978-0-07-011682-5, 2001. a
Pruppacher, H. and Klett, J.: Microphysics of clouds and precipitation, Reidel, Dordrecht, https://doi.org/10.1080/02786829808965531, 1997. a, b
Qiu, Y. and Molinero, V.: Why is it so difficult to identify the onset of ice premelting?, J. Phys. Chem., 9, 5179–5182, 2018. a
Roudsari, G., Lbadaoui-Darvas, M., Welti, A., Nenes, A., and Laaksonen, A.: The molecular scale mechanism of deposition ice nucleation on silver iodide, Environ. Sci. Atmos., 4, 243–251, https://doi.org/10.1039/D3EA00140G, 2024. a, b
Sorjamaa, R. and Laaksonen, A.: The effect of H2O adsorption on cloud drop activation of insoluble particles: a theoretical framework, Atmos. Chem. Phys., 7, 6175–6180, https://doi.org/10.5194/acp-7-6175-2007, 2007. a, b, c
Thürmer, K. and Nie, S.: Formation of hexagonal and cubic ice during low-temperature growth, P. Natl. Acad. Sci. USA, 110, 11757–11762, https://doi.org/10.1073/pnas.1303001110, 2013. a
Viisanen, Y., Lbadaoui-Darvas, M., Alvarez Piedehierro, A., Welti, A., Nenes, A., and Laaksonen, A.: Water vapor adsorption-desorption hysteresis due to clustering of water on nonporous surfaces, Langmuir, 40, 20311–20321, https://doi.org/10.1021/acs.langmuir.4c02950, 2024. a
Warring, S. L., Beatte, D. A., and McQuillan, J.: Surficial siloxane-to-silanol interconversion during room-temperature hydration/dehydration of amorphous silica films observed by ATR-IR and TIR-Raman spectroscopy, Langmuir, 32, 1568–1576, https://doi.org/10.1021/acs.langmuir.5b04506, 2016. a
Welti, A., Kanji, Z. A., Lüönd, F., Stetzer, O., and Lohmann, U.: Exploring the Mechanisms of Ice Nucleation on Kaolinite: From Deposition Nucleation to Condensation Freezing, J. Atmos. Sci, 71, 16–36, https://doi.org/10.1175/JAS-D-12-0252.1, 2014. a
Welti, A., Korhonen, K., Miettinen, P., Piedehierro, A. A., Viisanen, Y., Virtanen, A., and Laaksonen, A.: SPIN modification for low-temperature experiments, Atmos. Meas. Tech., 13, 7059–7067, https://doi.org/10.5194/amt-13-7059-2020, 2020. a
Yakobi-Hancock, J. D., Ladino, L. A., and Abbatt, J. P. D.: Feldspar minerals as efficient deposition ice nuclei, Atmos. Chem. Phys., 13, 11175–11185, https://doi.org/10.5194/acp-13-11175-2013, 2013. a
Yeşilbaş, M. and Boily, J.-F.: Thin Ice Films at Mineral Surfaces, J. Phys. Chem. Lett., 7, 2849–2855, https://doi.org/10.1021/acs.jpclett.6b01037, 2016. a
Zimmermann, F., Weinbruch, S., Schütz, L., Hofmann, H., Ebert, M., Kandler, K., and Worringen, A.: Ice nucleation properties of the most abundant mineral dust phases, J. Geophys. Res., 113, D23204, https://doi.org/10.1029/2008JD010655, 2008. a
Short summary
The mechanisms of ice nucleation at temperatures below 235 K have remained unclear for the past century. We suggest that ice nucleation is caused by the freezing of water adsorbed on aerosol surfaces. To test this hypothesis, we derived theoretical equations to predict the exact atmospheric conditions under which ice nucleation occurs. Our predictions agree well with experiments. The new theory thus provides a basis for an improved description of ice nucleation in the atmosphere.
The mechanisms of ice nucleation at temperatures below 235 K have remained unclear for the past...
Altmetrics
Final-revised paper
Preprint