Articles | Volume 25, issue 20
https://doi.org/10.5194/acp-25-13995-2025
© 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-25-13995-2025
© Author(s) 2025. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
28 Oct 2025
Research article |
| 28 Oct 2025
| 28 Oct 2025
Prior heterogeneous ice nucleation events shape homogeneous freezing during the evolution of synoptic cirrus
Kasper Juurikkala
CORRESPONDING AUTHOR
Finnish Meteorological Institute, 00560 Helsinki, Finland
Department of Physics, University of Helsinki, Helsinki, 00014, Finland
Christina J. Williamson
Finnish Meteorological Institute, 00560 Helsinki, Finland
Institute for Atmospheric and Earth System Research/Physics, University of Helsinki, Helsinki, 00014, Finland
Karl D. Froyd
Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, Colorado 80309, USA
Air Innova Research and Consulting, Boulder, CO 80305, USA
Jonathan Dean-Day
Bay Area Environmental Research Insititute, Moffett Field, CA 94035, USA
Ari Laaksonen
Finnish Meteorological Institute, 00560 Helsinki, Finland
Department of Technical Physics, University of Eastern Finland, 70211 Kuopio, Finland
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Aino Ovaska, Elio Rauth, Daniel Holmberg, Paulo Artaxo, John Backman, Benjamin Bergmans, Don Collins, Marco Aurélio Franco, Shahzad Gani, Roy M. Harrison, Rakesh 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, 3, 589–618, https://doi.org/10.5194/ar-3-589-2025, https://doi.org/10.5194/ar-3-589-2025, 2025
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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.
Abby Sebol, Glenn Wolfe, Timothy Canty, Jason St. Clair, Erin Delaria, Jennifer Kaiser, Nidhi Desai, Andrew Rollins, Eleanor Waxman, Kristen Zuraski, Bryan Place, Apoorva Pandey, Akanksha Singh, Allison Ring, Charles Gatebe, and Jonathan Dean-Day
EGUsphere, https://doi.org/10.5194/egusphere-2025-5261, https://doi.org/10.5194/egusphere-2025-5261, 2025
This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
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Ground-based spectrometers measuring HCHO and NO2 were compared to airborne in situ observations in the Summer 2023. Total column HCHO is within uncertainty, but with high biases near the surface. NO2 results are highly sensitive to the viewing angle of the ground monitor which must be considered during validation studies. Spectrometers in NYC show good agreement with a geostationary satellite on clear-sky days. Further quantified uncertainty for the monitors is necessary.
Larissa Lacher, A. Gannet Hallar, Ian B. McCubbin, Joey Bail, Karl D. Froyd, Justin Jacquot, Xiaoli Shen, Christopher Rapp, Ottmar Möhler, and Daniel Cziczo
EGUsphere, https://doi.org/10.5194/egusphere-2025-4492, https://doi.org/10.5194/egusphere-2025-4492, 2025
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We observe a trend of increasing ice-nucleating particle (INP) concentration in spring in the Rocky Mountains, related to regional dust emissions that may intensify with climate change. Additionally, super-micrometer particles were found as the most important contributors to the INP population. This finding was partly enabled by a novel setup of the Portable Ice Nucleation Experiment (PINE), coupled with a pumped-counterflow virtual impactor allowing for direct analysis of INP properties.
Ari Laaksonen, Golnaz Roudsari, Ana A. Piedehierro, and André Welti
Atmos. Chem. Phys., 25, 11317–11332, https://doi.org/10.5194/acp-25-11317-2025, https://doi.org/10.5194/acp-25-11317-2025, 2025
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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.
Xu-Cheng He, Nathan Luke Abraham, Han Ding, Maria R. Russo, Daniel P. Grosvenor, Yao Ge, Xuemei Wang, Anthony C. Jones, Pedro Campuzano-Jost, Benjamin Nault, Agnieszka Kupc, Donald Blake, Jose L. Jimenez, Christina J. Williamson, Kenneth S. Carslaw, James Weber, Alexander T. Archibald, and Hamish Gordon
EGUsphere, https://doi.org/10.5194/egusphere-2025-3700, https://doi.org/10.5194/egusphere-2025-3700, 2025
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Aerosols affect clouds and climate. However, current climate models still struggle to simulate them accurately. We used aircraft data from a global mission to evaluate how well the UK Earth System Model represents aerosols and their precursors. Our results show that the model misses key formation processes in clean ocean regions, suggesting that future improvements should focus on better representing how aerosols form naturally in the atmosphere.
Jasna V. Pittman, Bruce C. Daube, Steven C. Wofsy, Elliot L. Atlas, Maria A. Navarro, Eric J. Hintsa, Fred L. Moore, Geoff S. Dutton, James W. Elkins, Troy D. Thornberry, Andrew W. Rollins, Eric J. Jensen, Thaopaul Bui, Jonathan Dean-Day, and Leonhard Pfister
Atmos. Chem. Phys., 25, 7543–7562, https://doi.org/10.5194/acp-25-7543-2025, https://doi.org/10.5194/acp-25-7543-2025, 2025
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Biomass fires emit aerosols and precursors that can provide a novel environment for initiating stratospheric ozone loss. The Airborne Tropical TRopopause EXperiment campaign sampled the western Pacific, the dominant longitudes for surface air lofted by convection to enter the global stratosphere. Aircraft measurements over multiple flights revealed persistent layers of biomass burning pollutants entering the lower stratosphere and originating from fires as far away as Africa and Indonesia.
Paul J. DeMott, Jessica A. Mirrielees, Sarah Suda Petters, Daniel J. Cziczo, Markus D. Petters, Heinz G. Bingemer, Thomas C. J. Hill, Karl Froyd, Sarvesh Garimella, A. Gannet Hallar, Ezra J. T. Levin, Ian B. McCubbin, Anne E. Perring, Christopher N. Rapp, Thea Schiebel, Jann Schrod, Kaitlyn J. Suski, Daniel Weber, Martin J. Wolf, Maria Zawadowicz, Jake Zenker, Ottmar Möhler, and Sarah D. Brooks
Atmos. Meas. Tech., 18, 639–672, https://doi.org/10.5194/amt-18-639-2025, https://doi.org/10.5194/amt-18-639-2025, 2025
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The Fifth International Ice Nucleation Workshop Phase 3 (FIN-03) compared the ambient atmospheric performance of ice-nucleating particle (INP) measuring systems and explored general methods for discerning atmospheric INP compositions. Mirroring laboratory results, INP concentrations agreed within 5–10 factors. Measurements of total aerosol properties and investigations of INP compositions supported a dominant role of soil and plant organic aerosol elements as INPs during the study.
Gregory P. Schill, Karl D. Froyd, Daniel M. Murphy, Christina J. Williamson, Charles A. Brock, Tomás Sherwen, Mat J. Evans, Eric A. Ray, Eric C. Apel, Rebecca S. Hornbrook, Alan J. Hills, Jeff Peischl, Thomas B. Ryerson, Chelsea R. Thompson, Ilann Bourgeois, Donald R. Blake, Joshua P. DiGangi, and Glenn S. Diskin
Atmos. Chem. Phys., 25, 45–71, https://doi.org/10.5194/acp-25-45-2025, https://doi.org/10.5194/acp-25-45-2025, 2025
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Using single-particle mass spectrometry, we show that trace concentrations of bromine and iodine are ubiquitous in remote tropospheric aerosol and suggest that aerosols are an important part of the global reactive iodine budget. Comparisons to a global climate model with detailed iodine chemistry are favorable in the background atmosphere; however, the model cannot replicate our measurements near the ocean surface, in biomass burning plumes, and in the stratosphere.
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
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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.
Maya Abou-Ghanem, Daniel M. Murphy, Gregory P. Schill, Michael J. Lawler, and Karl D. Froyd
Atmos. Chem. Phys., 24, 8263–8275, https://doi.org/10.5194/acp-24-8263-2024, https://doi.org/10.5194/acp-24-8263-2024, 2024
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Using particle analysis by laser mass spectrometry, we examine vanadium-containing ship exhaust particles measured on NASA's DC-8 during the Atmospheric Tomography Mission (ATom). Our results reveal ship exhaust particles are sufficiently widespread in the marine atmosphere and experience atmospheric aging. Finally, we use laboratory calibrations to determine the vanadium, sulfate, and organic single-particle mass fractions of vanadium-containing ship exhaust particles.
Andrea E. Gordon, Cameron R. Homeyer, Jessica B. Smith, Rei Ueyama, Jonathan M. Dean-Day, Elliot L. Atlas, Kate Smith, Jasna V. Pittman, David S. Sayres, David M. Wilmouth, Apoorva Pandey, Jason M. St. Clair, Thomas F. Hanisco, Jennifer Hare, Reem A. Hannun, Steven Wofsy, Bruce C. Daube, and Stephen Donnelly
Atmos. Chem. Phys., 24, 7591–7608, https://doi.org/10.5194/acp-24-7591-2024, https://doi.org/10.5194/acp-24-7591-2024, 2024
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In situ airborne observations of ongoing tropopause-overshooting convection and an above-anvil cirrus plume from the 31 May 2022 flight of the Dynamics and Chemistry of the Summer Stratosphere (DCOTSS) field campaign are examined. Upper troposphere and lower stratosphere composition changes are evaluated along with possible contributing dynamical and physical processes. Measurements reveal multiple changes in air mass composition and stratospheric hydration throughout the flight.
Huisheng Bian, Mian Chin, Peter R. Colarco, Eric C. Apel, Donald R. Blake, Karl Froyd, Rebecca S. Hornbrook, Jose Jimenez, Pedro Campuzano Jost, Michael Lawler, Mingxu Liu, Marianne Tronstad Lund, Hitoshi Matsui, Benjamin A. Nault, Joyce E. Penner, Andrew W. Rollins, Gregory Schill, Ragnhild B. Skeie, Hailong Wang, Lu Xu, Kai Zhang, and Jialei Zhu
Atmos. Chem. Phys., 24, 1717–1741, https://doi.org/10.5194/acp-24-1717-2024, https://doi.org/10.5194/acp-24-1717-2024, 2024
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This work studies sulfur in the remote troposphere at global and seasonal scales using aircraft measurements and multi-model simulations. The goal is to understand the sulfur cycle over remote oceans, spread of model simulations, and observation–model discrepancies. Such an understanding and comparison with real observations are crucial to narrow down the uncertainties in model sulfur simulations and improve understanding of the sulfur cycle in atmospheric air quality, climate, and ecosystems.
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
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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.
Emma L. Yates, Laura T. Iraci, Susan S. Kulawik, Ju-Mee Ryoo, Josette E. Marrero, Caroline L. Parworth, Jason M. St. Clair, Thomas F. Hanisco, Thao Paul V. Bui, Cecilia S. Chang, and Jonathan M. Dean-Day
Earth Syst. Sci. Data, 15, 2375–2389, https://doi.org/10.5194/essd-15-2375-2023, https://doi.org/10.5194/essd-15-2375-2023, 2023
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The Alpha Jet Atmospheric eXperiment (AJAX) flew scientific flights between 2011 and 2018 providing measurements of carbon dioxide, methane, ozone, formaldehyde, water vapor and meteorological parameters over California and Nevada, USA. AJAX was a multi-year, multi-objective, multi-instrument program with a variety of sampling strategies resulting in an extensive dataset of interest to a wide variety of users. AJAX measurements have been published at https://asdc.larc.nasa.gov/project/AJAX.
Siying Lian, Luxi Zhou, Daniel M. Murphy, Karl D. Froyd, Owen B. Toon, and Pengfei Yu
Atmos. Chem. Phys., 22, 13659–13676, https://doi.org/10.5194/acp-22-13659-2022, https://doi.org/10.5194/acp-22-13659-2022, 2022
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Parameterizations of dust lifting and microphysical properties of dust in climate models are still subject to large uncertainty. Here we use a sectional aerosol climate model to investigate the global vertical distributions of the dust. Constrained by a suite of observations, the model suggests that, although North African dust dominates global dust mass loading at the surface, the relative contribution of Asian dust increases with altitude and becomes dominant in the upper troposphere.
Nicole A. June, Anna L. Hodshire, Elizabeth B. Wiggins, Edward L. Winstead, Claire E. Robinson, K. Lee Thornhill, Kevin J. Sanchez, Richard H. Moore, Demetrios Pagonis, Hongyu Guo, Pedro Campuzano-Jost, Jose L. Jimenez, Matthew M. Coggon, Jonathan M. Dean-Day, T. Paul Bui, Jeff Peischl, Robert J. Yokelson, Matthew J. Alvarado, Sonia M. Kreidenweis, Shantanu H. Jathar, and Jeffrey R. Pierce
Atmos. Chem. Phys., 22, 12803–12825, https://doi.org/10.5194/acp-22-12803-2022, https://doi.org/10.5194/acp-22-12803-2022, 2022
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The evolution of organic aerosol composition and size is uncertain due to variability within and between smoke plumes. We examine the impact of plume concentration on smoke evolution from smoke plumes sampled by the NASA DC-8 during FIREX-AQ. We find that observed organic aerosol and size distribution changes are correlated to plume aerosol mass concentrations. Additionally, coagulation explains the majority of the observed growth.
Meloë S. F. Kacenelenbogen, Qian Tan, Sharon P. Burton, Otto P. Hasekamp, Karl D. Froyd, Yohei Shinozuka, Andreas J. Beyersdorf, Luke Ziemba, Kenneth L. Thornhill, Jack E. Dibb, Taylor Shingler, Armin Sorooshian, Reed W. Espinosa, Vanderlei Martins, Jose L. Jimenez, Pedro Campuzano-Jost, Joshua P. Schwarz, Matthew S. Johnson, Jens Redemann, and Gregory L. Schuster
Atmos. Chem. Phys., 22, 3713–3742, https://doi.org/10.5194/acp-22-3713-2022, https://doi.org/10.5194/acp-22-3713-2022, 2022
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The impact of aerosols on Earth's radiation budget and human health is important and strongly depends on their composition. One desire of our scientific community is to derive the composition of the aerosol from satellite sensors. However, satellites observe aerosol optical properties (and not aerosol composition) based on remote sensing instrumentation. This study assesses how much aerosol optical properties can tell us about aerosol composition.
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
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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.
Li Zhang, Georg A. Grell, Stuart A. McKeen, Ravan Ahmadov, Karl D. Froyd, and Daniel Murphy
Geosci. Model Dev., 15, 467–491, https://doi.org/10.5194/gmd-15-467-2022, https://doi.org/10.5194/gmd-15-467-2022, 2022
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Applying the chemistry package from WRF-Chem into the Flow-following finite-volume Icosahedra Model, we essentially make it possible to explore the importance of different levels of complexity in gas and aerosol chemistry, as well as in physics parameterizations, for the interaction processes in global modeling systems. The model performance validated by the Atmospheric Tomography Mission aircraft measurements in summer 2016 shows good performance in capturing the aerosol and gas-phase tracers.
Charles A. Brock, Karl D. Froyd, Maximilian Dollner, Christina J. Williamson, Gregory Schill, Daniel M. Murphy, Nicholas J. Wagner, Agnieszka Kupc, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jason C. Schroder, Douglas A. Day, Derek J. Price, Bernadett Weinzierl, Joshua P. Schwarz, Joseph M. Katich, Siyuan Wang, Linghan Zeng, Rodney Weber, Jack Dibb, Eric Scheuer, Glenn S. Diskin, Joshua P. DiGangi, ThaoPaul Bui, Jonathan M. Dean-Day, Chelsea R. Thompson, Jeff Peischl, Thomas B. Ryerson, Ilann Bourgeois, Bruce C. Daube, Róisín Commane, and Steven C. Wofsy
Atmos. Chem. Phys., 21, 15023–15063, https://doi.org/10.5194/acp-21-15023-2021, https://doi.org/10.5194/acp-21-15023-2021, 2021
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The Atmospheric Tomography Mission was an airborne study that mapped the chemical composition of the remote atmosphere. From this, we developed a comprehensive description of aerosol properties that provides a unique, global-scale dataset against which models can be compared. The data show the polluted nature of the remote atmosphere in the Northern Hemisphere and quantify the contributions of sea salt, dust, soot, biomass burning particles, and pollution particles to the haziness of the sky.
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
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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.
Christina J. Williamson, Agnieszka Kupc, Andrew Rollins, Jan Kazil, Karl D. Froyd, Eric A. Ray, Daniel M. Murphy, Gregory P. Schill, Jeff Peischl, Chelsea Thompson, Ilann Bourgeois, Thomas B. Ryerson, Glenn S. Diskin, Joshua P. DiGangi, Donald R. Blake, Thao Paul V. Bui, Maximilian Dollner, Bernadett Weinzierl, and Charles A. Brock
Atmos. Chem. Phys., 21, 9065–9088, https://doi.org/10.5194/acp-21-9065-2021, https://doi.org/10.5194/acp-21-9065-2021, 2021
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Aerosols in the stratosphere influence climate by scattering and absorbing sunlight and through chemical reactions occurring on the particles’ surfaces. We observed more nucleation mode aerosols (small aerosols, with diameters below 12 nm) in the mid- and high-latitude lowermost stratosphere (8–13 km) in the Northern Hemisphere (NH) than in the Southern Hemisphere. The most likely cause of this is aircraft emissions, which are concentrated in the NH at similar altitudes to our observations.
Daniel M. Murphy, Karl D. Froyd, Ilann Bourgeois, Charles A. Brock, Agnieszka Kupc, Jeff Peischl, Gregory P. Schill, Chelsea R. Thompson, Christina J. Williamson, and Pengfei Yu
Atmos. Chem. Phys., 21, 8915–8932, https://doi.org/10.5194/acp-21-8915-2021, https://doi.org/10.5194/acp-21-8915-2021, 2021
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New measurements in the lower stratosphere highlight differences between particles that originated in the troposphere or the stratosphere. The stratospheric-origin particles have relatively large radiative effects because they are at nearly the optimum diameter for light scattering. The tropospheric particles contribute significantly to surface area. These and other chemical and physical properties are then extended to study the implications if material were to be added to the stratosphere.
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
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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.
Agnieszka Kupc, Christina J. Williamson, Anna L. Hodshire, Jan Kazil, Eric Ray, T. Paul Bui, Maximilian Dollner, Karl D. Froyd, Kathryn McKain, Andrew Rollins, Gregory P. Schill, Alexander Thames, Bernadett B. Weinzierl, Jeffrey R. Pierce, and Charles A. Brock
Atmos. Chem. Phys., 20, 15037–15060, https://doi.org/10.5194/acp-20-15037-2020, https://doi.org/10.5194/acp-20-15037-2020, 2020
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Tropical upper troposphere over the Atlantic and Pacific oceans is a major source region of new particles. These particles are associated with the outflow from deep convection. We investigate the processes that govern the formation of these particles and their initial growth and show that none of the formation schemes commonly used in global models are consistent with observations. Using newer schemes indicates that organic compounds are likely important as nucleating and initial growth agents.
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Short summary
This study uses Large Eddy Simulations (LES) to investigate synoptic cirrus clouds from NASA’s Mid-latitude Airborne Cirrus Properties Experiment (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.
This study uses Large Eddy Simulations (LES) to investigate synoptic cirrus clouds from NASA’s...
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