Articles | Volume 26, issue 12
https://doi.org/10.5194/acp-26-9221-2026
© Author(s) 2026. 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-26-9221-2026
© Author(s) 2026. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
The impact of aerosol mixing state on immersion freezing: insights from classical nucleation theory and particle-resolved simulations
Wenhan Tang
CORRESPONDING AUTHOR
Department of Climate, Meteorology, and Atmospheric Sciences, University of Illinois Urbana-Champaign, Urbana, Illinois, USA
Sylwester Arabas
Faculty of Physics and Applied Computer Science, AGH University of Krakow, Kraków, Poland
Jeffrey H. Curtis
Department of Climate, Meteorology, and Atmospheric Sciences, University of Illinois Urbana-Champaign, Urbana, Illinois, USA
Daniel A. Knopf
School of Marine and Atmospheric Sciences, Stony Brook University, Stony Brook, New York, USA
Matthew West
Department of Mechanical Science and Engineering, University of Illinois Urbana-Champaign, Urbana, Illinois, USA
Department of Climate, Meteorology, and Atmospheric Sciences, University of Illinois Urbana-Champaign, Urbana, Illinois, USA
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Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2022-428, https://doi.org/10.5194/essd-2022-428, 2022
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Homogeneous freezing describes the spontaneous freezing of supercooled droplets, with the probability depending on temperature, droplet size, and elapsed time. Droplets freeze across a range of temperatures rather than all at once, and faster updrafts and larger droplets lead to freezing at warmer temperatures. Once some droplets freeze, the growing ice crystals deplete the surrounding vapour, causing the remaining droplets to evaporate. This affects the number of ice crystals in the cloud.
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Atmos. Chem. Phys., 26, 4863–4883, https://doi.org/10.5194/acp-26-4863-2026, https://doi.org/10.5194/acp-26-4863-2026, 2026
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Airborne particles affect clouds, climate, and air quality, but it is difficult to determine how their chemical components are mixed within individual particles. We tested a method that estimates this mixing from water-uptake measurements using detailed computer simulations. The method works well in many cases, but can overestimate particle mixing when moderately water-attracting material exists in separate particle types. We then applied this uncertainty framework to long-term observations.
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Geosci. Model Dev., 19, 1581–1617, https://doi.org/10.5194/gmd-19-1581-2026, https://doi.org/10.5194/gmd-19-1581-2026, 2026
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The role of Arctic clouds in the regional climate remains uncertain due to insufficient understanding of the amount of liquid droplets and ice crystals present in these clouds. An aerosol-cloud model is employed to examine the role of different aerosol types and freezing parameterizations on the number of ice crystals. The choice of freezing parameterization significantly changes the number of ice crystals impacting the interpretation of the evolution and warming effect of Arctic clouds.
Oscar H. Díaz-Ibarra, Samuel G. Frederick, Jeffrey H. Curtis, Zachary D'Aquino, Peter A. Bosler, Lekha Patel, Cosmin Safta, Matthew West, and Nicole Riemer
Geosci. Model Dev., 19, 1281–1299, https://doi.org/10.5194/gmd-19-1281-2026, https://doi.org/10.5194/gmd-19-1281-2026, 2026
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We developed TChem-atm, a new open-source tool for simulating atmospheric chemistry and aerosols. As models become more detailed, traditional methods are too slow. TChem-atm runs on both standard processors and graphics processors, making these simulations faster and more efficient. The tool provides a foundation for next-generation models that improve predictions of air quality and climate.
Cristofer Jimenez, Albert Ansmann, Kevin Ohneiser, Hannes Griesche, Ronny Engelmann, Martin Radenz, Julian Hofer, Dietrich Althausen, Daniel A. Knopf, Sandro Dahlke, Johannes Bühl, Holger Baars, Patric Seifert, and Ulla Wandinger
Atmos. Chem. Phys., 25, 12955–12981, https://doi.org/10.5194/acp-25-12955-2025, https://doi.org/10.5194/acp-25-12955-2025, 2025
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We studied the water and ice phases of Arctic mixed-phase clouds (MPCs) using dual FOV polarization lidar and Doppler radar on board Polarstern during the MOSAiC expedition. Two long-lasting Arctic MPCs and year-round statistics show persistent droplet activation and dominant immersion freezing, indicating well-filled cloud condensation nuclei and ice-nucleating particle reservoirs. These findings help explain MPC longevity and may improve cloud life cycle representation in weather and climate models.
Albert Ansmann, Cristofer Jimenez, Daniel A. Knopf, Johanna Roschke, Johannes Bühl, Kevin Ohneiser, and Ronny Engelmann
Atmos. Chem. Phys., 25, 4867–4884, https://doi.org/10.5194/acp-25-4867-2025, https://doi.org/10.5194/acp-25-4867-2025, 2025
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In this study, we focus on the potential impact of wildfire smoke on cirrus formation. Aerosol and cirrus observations with lidar and radar during the MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition, presented in the companion paper (Ansmann et al., 2025), are closely linked to comprehensive modeling of ice nucleation in cirrus evolution processes, presented in this article. A clear impact of wildfire smoke on cirrus formation was found.
Albert Ansmann, Cristofer Jimenez, Johanna Roschke, Johannes Bühl, Kevin Ohneiser, Ronny Engelmann, Martin Radenz, Hannes Griesche, Julian Hofer, Dietrich Althausen, Daniel A. Knopf, Sandro Dahlke, Tom Gaudek, Patric Seifert, and Ulla Wandinger
Atmos. Chem. Phys., 25, 4847–4866, https://doi.org/10.5194/acp-25-4847-2025, https://doi.org/10.5194/acp-25-4847-2025, 2025
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In this study, we focus on the potential impact of wildfire smoke on cirrus formation. For the first time, state-of-the-art aerosol and cirrus observations with lidar and radar, presented in this paper (Part 1 of a series of two articles), are closely linked to the comprehensive modeling of gravity-wave-induced ice nucleation in cirrus evolution processes, presented in a companion paper (Part 2). We found a clear impact of wildfire smoke on cirrus evolution.
Zhouyang Zhang, Jiandong Wang, Jiaping Wang, Nicole Riemer, Chao Liu, Yuzhi Jin, Zeyuan Tian, Jing Cai, Yueyue Cheng, Ganzhen Chen, Bin Wang, Shuxiao Wang, and Aijun Ding
Atmos. Chem. Phys., 25, 1869–1881, https://doi.org/10.5194/acp-25-1869-2025, https://doi.org/10.5194/acp-25-1869-2025, 2025
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Black carbon (BC) exerts notable warming effects. We use a particle-resolved model to investigate the long-term behavior of the BC mixing state, revealing its compositions, coating thickness distribution, and optical properties all stabilize with a characteristic time of less than 1 d. This study can effectively simplify the description of the BC mixing state, which facilitates the precise assessment of the optical properties of BC aerosols in global and chemical transport models.
Jeffrey H. Curtis, Nicole Riemer, and Matthew West
Geosci. Model Dev., 17, 8399–8420, https://doi.org/10.5194/gmd-17-8399-2024, https://doi.org/10.5194/gmd-17-8399-2024, 2024
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This paper introduces a numerical method for simulating particle-based aerosol transport in atmospheric models. We detail the various numerical properties of the advection order method and demonstrate its implementation in a 3D weather prediction model (WRF) for the first time. Particle-based techniques improve the accuracy of aerosol size and composition predictions, which are key for aerosol–cloud and aerosol–radiation interactions.
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Atmos. Chem. Phys., 24, 3445–3528, https://doi.org/10.5194/acp-24-3445-2024, https://doi.org/10.5194/acp-24-3445-2024, 2024
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Rodanthi-Elisavet Mamouri, Albert Ansmann, Kevin Ohneiser, Daniel A. Knopf, Argyro Nisantzi, Johannes Bühl, Ronny Engelmann, Annett Skupin, Patric Seifert, Holger Baars, Dragos Ene, Ulla Wandinger, and Diofantos Hadjimitsis
Atmos. Chem. Phys., 23, 14097–14114, https://doi.org/10.5194/acp-23-14097-2023, https://doi.org/10.5194/acp-23-14097-2023, 2023
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For the first time, rather clear evidence is found that wildfire smoke particles can trigger strong cirrus formation. This finding is of importance because intensive and large wildfires may occur increasingly often in the future as climate change proceeds. Based on lidar observations in Cyprus in autumn 2020, we provide detailed insight into the cirrus formation at the tropopause in the presence of aged wildfire smoke (here, 8–9 day old Californian wildfire smoke).
Albert Ansmann, Kevin Ohneiser, Ronny Engelmann, Martin Radenz, Hannes Griesche, Julian Hofer, Dietrich Althausen, Jessie M. Creamean, Matthew C. Boyer, Daniel A. Knopf, Sandro Dahlke, Marion Maturilli, Henriette Gebauer, Johannes Bühl, Cristofer Jimenez, Patric Seifert, and Ulla Wandinger
Atmos. Chem. Phys., 23, 12821–12849, https://doi.org/10.5194/acp-23-12821-2023, https://doi.org/10.5194/acp-23-12821-2023, 2023
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The 1-year MOSAiC (2019–2020) expedition with the German ice breaker Polarstern was the largest polar field campaign ever conducted. The Polarstern, with our lidar aboard, drifted with the pack ice north of 85° N for more than 7 months (October 2019 to mid-May 2020). We measured the full annual cycle of aerosol conditions in terms of aerosol optical and cloud-process-relevant properties. We observed a strong contrast between polluted winter and clean summer aerosol conditions.
Daniel A. Knopf, Peiwen Wang, Benny Wong, Jay M. Tomlin, Daniel P. Veghte, Nurun N. Lata, Swarup China, Alexander Laskin, Ryan C. Moffet, Josephine Y. Aller, Matthew A. Marcus, and Jian Wang
Atmos. Chem. Phys., 23, 8659–8681, https://doi.org/10.5194/acp-23-8659-2023, https://doi.org/10.5194/acp-23-8659-2023, 2023
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Ambient particle populations and associated ice-nucleating particles (INPs)
were examined from particle samples collected on board aircraft in the marine
boundary layer and free troposphere in the eastern North Atlantic during
summer and winter. Chemical imaging shows distinct differences in the
particle populations seasonally and with sampling altitudes, which are
reflected in the INP types. Freezing parameterizations are derived for
implementation in cloud-resolving and climate models.
Emily de Jong, John Ben Mackay, Oleksii Bulenok, Anna Jaruga, and Sylwester Arabas
Geosci. Model Dev., 16, 4193–4211, https://doi.org/10.5194/gmd-16-4193-2023, https://doi.org/10.5194/gmd-16-4193-2023, 2023
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In clouds, collisional breakup occurs when two colliding droplets splinter into new, smaller fragments. Particle-based modeling approaches often do not represent breakup because of the computational demands of creating new droplets. We present a particle-based breakup method that preserves the computational efficiency of these methods. In a series of simple demonstrations, we show that this representation alters cloud processes in reasonable and expected ways.
Sudipta Ghosh, Sagnik Dey, Sushant Das, Nicole Riemer, Graziano Giuliani, Dilip Ganguly, Chandra Venkataraman, Filippo Giorgi, Sachchida Nand Tripathi, Srikanthan Ramachandran, Thazhathakal Ayyappen Rajesh, Harish Gadhavi, and Atul Kumar Srivastava
Geosci. Model Dev., 16, 1–15, https://doi.org/10.5194/gmd-16-1-2023, https://doi.org/10.5194/gmd-16-1-2023, 2023
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Accurate representation of aerosols in climate models is critical for minimizing the uncertainty in climate projections. Here, we implement region-specific emission fluxes and a more accurate scheme for carbonaceous aerosol ageing processes in a regional climate model (RegCM4) and show that it improves model performance significantly against in situ, reanalysis, and satellite data over the Indian subcontinent. We recommend improving the model performance before using them for climate studies.
Wenxiu Zhang, Di Liu, Hanqin Tian, Naiqin Pan, Ruqi Yang, Wenhan Tang, Jia Yang, Fei Lu, Buddhi Dayananda, Han Mei, Siyuan Wang, and Hao Shi
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2022-428, https://doi.org/10.5194/essd-2022-428, 2022
Manuscript not accepted for further review
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High temporal resolution surface ozone concentration data is still lacking in China, so we used deep learning to generate hourly surface ozone data (HrSOD) during 2005–2020 across China. HrSOD showed that surface O3 in China tended to increase from 2016 to 2019, despite a decrease in 2020. HrSOD had high spatial and temporal accuracies, long time ranges and high temporal resolution, enabling it to be easily converted to various evaluation indicators for ecosystem and human health assessments.
Albert Ansmann, Kevin Ohneiser, Alexandra Chudnovsky, Daniel A. Knopf, Edwin W. Eloranta, Diego Villanueva, Patric Seifert, Martin Radenz, Boris Barja, Félix Zamorano, Cristofer Jimenez, Ronny Engelmann, Holger Baars, Hannes Griesche, Julian Hofer, Dietrich Althausen, and Ulla Wandinger
Atmos. Chem. Phys., 22, 11701–11726, https://doi.org/10.5194/acp-22-11701-2022, https://doi.org/10.5194/acp-22-11701-2022, 2022
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For the first time we present a systematic study on the impact of wildfire smoke on ozone depletion in the Arctic (2020) and Antarctic stratosphere (2020, 2021). Two major fire events in Siberia and Australia were responsible for the observed record-breaking stratospheric smoke pollution. Our analyses were based on lidar observations of smoke parameters (Polarstern, Punta Arenas) and NDACC Arctic and Antarctic ozone profiles as well as on Antarctic OMI satellite observations of column ozone.
Yu Yao, Jeffrey H. Curtis, Joseph Ching, Zhonghua Zheng, and Nicole Riemer
Atmos. Chem. Phys., 22, 9265–9282, https://doi.org/10.5194/acp-22-9265-2022, https://doi.org/10.5194/acp-22-9265-2022, 2022
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Investigating the impacts of aerosol mixing state on aerosol optical properties has a long history from both the modeling and experimental perspective. In this study, we used particle-resolved simulations as a benchmark to determine the error in optical properties when using simplified aerosol representations. We found that errors in single scattering albedo due to the internal mixture assumptions can have substantial effects on calculating aerosol direct radiative forcing.
Kevin Ohneiser, Albert Ansmann, Bernd Kaifler, Alexandra Chudnovsky, Boris Barja, Daniel A. Knopf, Natalie Kaifler, Holger Baars, Patric Seifert, Diego Villanueva, Cristofer Jimenez, Martin Radenz, Ronny Engelmann, Igor Veselovskii, and Félix Zamorano
Atmos. Chem. Phys., 22, 7417–7442, https://doi.org/10.5194/acp-22-7417-2022, https://doi.org/10.5194/acp-22-7417-2022, 2022
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We present and discuss 2 years of long-term lidar observations of the largest stratospheric perturbation by wildfire smoke ever observed. The smoke originated from the record-breaking Australian fires in 2019–2020 and affects climate conditions and even the ozone layer in the Southern Hemisphere. The obvious link between dense smoke occurrence in the stratosphere and strong ozone depletion found in the Arctic and in the Antarctic in 2020 can be regarded as a new aspect of climate change.
Michael A. Olesik, Jakub Banaśkiewicz, Piotr Bartman, Manuel Baumgartner, Simon Unterstrasser, and Sylwester Arabas
Geosci. Model Dev., 15, 3879–3899, https://doi.org/10.5194/gmd-15-3879-2022, https://doi.org/10.5194/gmd-15-3879-2022, 2022
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In systems such as atmospheric clouds, droplets undergo growth through condensation of vapor. The broadness of the resultant size spectrum of droplets influences precipitation likelihood and the radiative properties of clouds. One of the inherent limitations of simulations of the problem is the so-called numerical diffusion causing overestimation of the spectrum width, hence the term numerical broadening. In the paper, we take a closer look at one of the algorithms used in this context: MPDATA.
Matthew L. Dawson, Christian Guzman, Jeffrey H. Curtis, Mario Acosta, Shupeng Zhu, Donald Dabdub, Andrew Conley, Matthew West, Nicole Riemer, and Oriol Jorba
Geosci. Model Dev., 15, 3663–3689, https://doi.org/10.5194/gmd-15-3663-2022, https://doi.org/10.5194/gmd-15-3663-2022, 2022
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Progress in identifying complex, mixed-phase physicochemical processes has resulted in an advanced understanding of the evolution of atmospheric systems but has also introduced a level of complexity that few atmospheric models were designed to handle. We present a flexible treatment for multiphase chemical processes for models of diverse scale, from box up to global models. This enables users to build a customized multiphase mechanism that is accessible to a much wider community.
Daniel A. Knopf, Joseph C. Charnawskas, Peiwen Wang, Benny Wong, Jay M. Tomlin, Kevin A. Jankowski, Matthew Fraund, Daniel P. Veghte, Swarup China, Alexander Laskin, Ryan C. Moffet, Mary K. Gilles, Josephine Y. Aller, Matthew A. Marcus, Shira Raveh-Rubin, and Jian Wang
Atmos. Chem. Phys., 22, 5377–5398, https://doi.org/10.5194/acp-22-5377-2022, https://doi.org/10.5194/acp-22-5377-2022, 2022
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Marine boundary layer aerosols collected in the remote region of the eastern North Atlantic induce immersion freezing and deposition ice nucleation under typical mixed-phase and cirrus cloud conditions. Corresponding ice nucleation parameterizations for model applications have been derived. Chemical imaging of ambient aerosol and ice-nucleating particles demonstrates that the latter is dominated by sea salt and organics while also representing a major particle type in the particle population.
Jay M. Tomlin, Kevin A. Jankowski, Daniel P. Veghte, Swarup China, Peiwen Wang, Matthew Fraund, Johannes Weis, Guangjie Zheng, Yang Wang, Felipe Rivera-Adorno, Shira Raveh-Rubin, Daniel A. Knopf, Jian Wang, Mary K. Gilles, Ryan C. Moffet, and Alexander Laskin
Atmos. Chem. Phys., 21, 18123–18146, https://doi.org/10.5194/acp-21-18123-2021, https://doi.org/10.5194/acp-21-18123-2021, 2021
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Analysis of individual atmospheric particles shows that aerosol transported from North America during meteorological dry intrusion episodes may have a substantial impact on the mixing state and particle-type population over the mid-Atlantic, as organic contribution and particle-type diversity are significantly enhanced during these periods. These observations need to be considered in current atmospheric models.
Zhonghua Zheng, Matthew West, Lei Zhao, Po-Lun Ma, Xiaohong Liu, and Nicole Riemer
Atmos. Chem. Phys., 21, 17727–17741, https://doi.org/10.5194/acp-21-17727-2021, https://doi.org/10.5194/acp-21-17727-2021, 2021
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Aerosol mixing state is an important emergent property that affects aerosol radiative forcing and aerosol–cloud interactions, but it has not been easy to constrain this property globally. We present a framework for evaluating the error in aerosol mixing state induced by aerosol representation assumptions, which is one of the important contributors to structural uncertainty in aerosol models. Our study provides insights into potential improvements to model process representation for aerosols.
Daniel A. Knopf and Markus Ammann
Atmos. Chem. Phys., 21, 15725–15753, https://doi.org/10.5194/acp-21-15725-2021, https://doi.org/10.5194/acp-21-15725-2021, 2021
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Adsorption on and desorption of gas molecules from solid or liquid surfaces or interfaces represent the initial interaction of gas-to-condensed-phase processes that can define the physicochemical evolution of the condensed phase. We apply a thermodynamic and microscopic treatment of these multiphase processes to evaluate how adsorption and desorption rates and surface accommodation depend on the choice of adsorption model and standard states with implications for desorption energy and lifetimes.
Yang Wang, Guangjie Zheng, Michael P. Jensen, Daniel A. Knopf, Alexander Laskin, Alyssa A. Matthews, David Mechem, Fan Mei, Ryan Moffet, Arthur J. Sedlacek, John E. Shilling, Stephen Springston, Amy Sullivan, Jason Tomlinson, Daniel Veghte, Rodney Weber, Robert Wood, Maria A. Zawadowicz, and Jian Wang
Atmos. Chem. Phys., 21, 11079–11098, https://doi.org/10.5194/acp-21-11079-2021, https://doi.org/10.5194/acp-21-11079-2021, 2021
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This paper reports the vertical profiles of trace gas and aerosol properties over the eastern North Atlantic, a region of persistent but diverse subtropical marine boundary layer (MBL) clouds. We examined the key processes that drive the cloud condensation nuclei (CCN) population and how it varies with season and synoptic conditions. This study helps improve the model representation of the aerosol processes in the remote MBL, reducing the simulated aerosol indirect effects.
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Short summary
We studied how aerosol particles help form ice in clouds. Using new theory and detailed computer simulations, we found that the way different materials are mixed within these particles has a strong impact on how much ice forms. When ice-forming material is spread across all particles, more droplets freeze than when it is only in a few. This result means that to better predict clouds and climate, models need to account for how particle materials are mixed.
We studied how aerosol particles help form ice in clouds. Using new theory and detailed computer...
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