Articles | Volume 13, issue 17
https://doi.org/10.5194/acp-13-9097-2013
© Author(s) 2013. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-13-9097-2013
© Author(s) 2013. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
10 Sep 2013
Research article |
| 10 Sep 2013
Laboratory studies of immersion and deposition mode ice nucleation of ozone aged mineral dust particles
Z. A. Kanji
Institute for Atmospheric and Climate Sciences, ETH, Zurich, 8092, Switzerland
now at: Air Quality Research Division, Environment Canada, Toronto, ON, M3H 5T4, Canada
Institute for Atmospheric and Climate Sciences, ETH, Zurich, 8092, Switzerland
C. Chou
Institute for Atmospheric and Climate Sciences, ETH, Zurich, 8092, Switzerland
now at: Science and Technology Research Institute, University of Hertfordshire, College Lane, AL10 9AB, Hatfield, UK
O. Stetzer
Institute for Atmospheric and Climate Sciences, ETH, Zurich, 8092, Switzerland
U. Lohmann
Institute for Atmospheric and Climate Sciences, ETH, Zurich, 8092, Switzerland
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Special microscopic particles called ice-nucleating particles (INPs) are essential for ice crystals to form in the atmosphere. INPs are sparse and their atmospheric concentration and properties are not well understood. Mineral dust particles make up a significant fraction of INPs but how much remains unknown. Here, we address this knowledge gap by studying periods when mineral particles are present in large quantities at a mountaintop station in central Europe.
Larissa Lacher, Hans-Christian Clemen, Xiaoli Shen, Stephan Mertes, Martin Gysel-Beer, Alireza Moallemi, Martin Steinbacher, Stephan Henne, Harald Saathoff, Ottmar Möhler, Kristina Höhler, Thea Schiebel, Daniel Weber, Jann Schrod, Johannes Schneider, and Zamin A. Kanji
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We investigate ice-nucleating particle properties at Jungfraujoch during the 2017 joint INUIT/CLACE field campaign, to improve the knowledge about those rare particles in a cloud-relevant environment. By quantifying ice-nucleating particles in parallel to single-particle mass spectrometry measurements, we find that mineral dust and aged sea spray particles are potential candidates for ice-nucleating particles. Our findings are supported by ice residual analysis and source region modeling.
Paraskevi Georgakaki, Aikaterini Bougiatioti, Jörg Wieder, Claudia Mignani, Fabiola Ramelli, Zamin A. Kanji, Jan Henneberger, Maxime Hervo, Alexis Berne, Ulrike Lohmann, and Athanasios Nenes
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Aerosol and cloud observations coupled with a droplet activation parameterization was used to investigate the aerosol–cloud droplet link in alpine mixed-phase clouds. Predicted droplet number, Nd, agrees with observations and never exceeds a characteristic “limiting droplet number”, Ndlim, which depends solely on σw. Nd becomes velocity limited when it is within 50 % of Ndlim. Identifying when dynamical changes control Nd variability is central for understanding aerosol–cloud interactions.
Claudia Mignani, Jörg Wieder, Michael A. Sprenger, Zamin A. Kanji, Jan Henneberger, Christine Alewell, and Franz Conen
Atmos. Chem. Phys., 21, 657–664, https://doi.org/10.5194/acp-21-657-2021, https://doi.org/10.5194/acp-21-657-2021, 2021
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Most precipitation above land starts with ice in clouds. It is promoted by extremely rare particles. Some ice-nucleating particles (INPs) cause cloud droplets to already freeze above −15°C, a temperature at which many clouds begin to snow. We found that the abundance of such INPs among other particles of similar size is highest in precipitating air masses and lowest when air carries desert dust. This brings us closer to understanding the interactions between land, clouds, and precipitation.
Cyril Brunner and Zamin A. Kanji
Atmos. Meas. Tech., 14, 269–293, https://doi.org/10.5194/amt-14-269-2021, https://doi.org/10.5194/amt-14-269-2021, 2021
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Subvisual microscopic particles in the atmosphere are needed to act as seeds for cloud droplets or ice crystals to form. The microscopic particles, called ice-nucleating particles (INPs), form ice crystals and are rare, and their properties are not well understood, in part because measuring them is challenging and time consuming, and to date has not been automated. Here, we present the first online instrument that can continuously and autonomously measure INP concentration at 243 K.
Robert O. David, Jonas Fahrni, Claudia Marcolli, Fabian Mahrt, Dominik Brühwiler, and Zamin A. Kanji
Atmos. Chem. Phys., 20, 9419–9440, https://doi.org/10.5194/acp-20-9419-2020, https://doi.org/10.5194/acp-20-9419-2020, 2020
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Ice crystal formation plays an important role in controlling the Earth's climate. However, the mechanisms responsible for ice formation in the atmosphere are still uncertain. Here we use surrogates for atmospherically relevant porous particles to determine the role of pore diameter and wettability on the ability of porous particles to nucleate ice in the atmosphere. Our results are consistent with the pore condensation and freeing mechanism.
Mikhail Paramonov, Saskia Drossaart van Dusseldorp, Ellen Gute, Jonathan P. D. Abbatt, Paavo Heikkilä, Jorma Keskinen, Xuemeng Chen, Krista Luoma, Liine Heikkinen, Liqing Hao, Tuukka Petäjä, and Zamin A. Kanji
Atmos. Chem. Phys., 20, 6687–6706, https://doi.org/10.5194/acp-20-6687-2020, https://doi.org/10.5194/acp-20-6687-2020, 2020
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Ice-nucleating particle (INP) measurements were performed in the boreal environment of southern Finland in the winter–spring of 2018. It was found that no single parameter could be used to predict the INP number concentration at the measurement location during the examined time period. It was also not possible to identify physical and chemical properties of ambient INPs despite the complexity of the instrumental set-up. Therefore, this paper addresses the necessity for future INP measurements.
Robert O. David, Maria Cascajo-Castresana, Killian P. Brennan, Michael Rösch, Nora Els, Julia Werz, Vera Weichlinger, Lin S. Boynton, Sophie Bogler, Nadine Borduas-Dedekind, Claudia Marcolli, and Zamin A. Kanji
Atmos. Meas. Tech., 12, 6865–6888, https://doi.org/10.5194/amt-12-6865-2019, https://doi.org/10.5194/amt-12-6865-2019, 2019
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Here we present the development and applicability of the DRoplet Ice Nuclei Counter Zurich (DRINCZ). DRINCZ allows for ice nuclei in the immersion mode to be quantified between 0 and -25 °C with an uncertainty of ±0.9 °C. Furthermore, we present a new method for assessing biases in drop-freezing apparatuses and cumulative ice-nucleating-particle concentrations from snow samples collected in the Austrian Alps at the Sonnblick Observatory.
Albert Ansmann, Rodanthi-Elisavet Mamouri, Johannes Bühl, Patric Seifert, Ronny Engelmann, Julian Hofer, Argyro Nisantzi, James D. Atkinson, Zamin A. Kanji, Berko Sierau, Mihalis Vrekoussis, and Jean Sciare
Atmos. Chem. Phys., 19, 15087–15115, https://doi.org/10.5194/acp-19-15087-2019, https://doi.org/10.5194/acp-19-15087-2019, 2019
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For the first time, a closure study of the relationship between the ice-nucleating particle concentration (INPC) and ice crystal number concentration (ICNC) in altocumulus and cirrus layers, solely based on ground-based active remote sensing, is presented. The closure studies were conducted in Cyprus. A focus was on altocumulus and cirrus layers which developed in pronounced Saharan dust layers. The closure studies show that heterogeneous ice nucleation can play a dominant role in ice formation.
Nadine Borduas-Dedekind, Rachele Ossola, Robert O. David, Lin S. Boynton, Vera Weichlinger, Zamin A. Kanji, and Kristopher McNeill
Atmos. Chem. Phys., 19, 12397–12412, https://doi.org/10.5194/acp-19-12397-2019, https://doi.org/10.5194/acp-19-12397-2019, 2019
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During atmospheric transport, dissolved organic matter (DOM) within aqueous aerosols undergoes photochemistry. We find that photochemical processing of DOM increases its ability to form cloud droplets but decreases its ability to form ice crystals over a simulated 4.6 days in the atmosphere. A photomineralization mechanism involving the loss of organic carbon and the production of organic acids, CO and CO2 explains the observed changes and affects the liquid-water-to-ice ratio in clouds.
André Welti, Ulrike Lohmann, and Zamin A. Kanji
Atmos. Chem. Phys., 19, 10901–10918, https://doi.org/10.5194/acp-19-10901-2019, https://doi.org/10.5194/acp-19-10901-2019, 2019
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The ice nucleation ability of singly immersed feldspar particles in suspended water droplets relevant for ice crystal formation under mixed-phase cloud conditions is presented. The effects of particle size, crystal structure, trace metal and mineralogical composition are discussed by testing up to five different diameters in the submicron range and nine different feldspar samples at conditions relevant for ice nucleation in mixed-phase clouds.
Fabian Mahrt, Jörg Wieder, Remo Dietlicher, Helen R. Smith, Chris Stopford, and Zamin A. Kanji
Atmos. Meas. Tech., 12, 3183–3208, https://doi.org/10.5194/amt-12-3183-2019, https://doi.org/10.5194/amt-12-3183-2019, 2019
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A new instrument, the High Speed Particle Phase Discriminator (PPD-HS), is presented, with the goal of quantifying liquid and ice fraction in conditions relevant for mixed-phase clouds. PPD-HS captures the near-forward spatial intensity distribution of scattered light on a single particle basis. Symmetry analysis of the scattering pattern is used to determine the shape of the particles, with cloud droplets and ice crystals producing symmetrical and asymmetrical scattering patterns, respectively.
Zamin A. Kanji, Ryan C. Sullivan, Monika Niemand, Paul J. DeMott, Anthony J. Prenni, Cédric Chou, Harald Saathoff, and Ottmar Möhler
Atmos. Chem. Phys., 19, 5091–5110, https://doi.org/10.5194/acp-19-5091-2019, https://doi.org/10.5194/acp-19-5091-2019, 2019
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The ice nucleation ability of two natural desert dusts coated with a proxy of secondary organic aerosol is presented for temperatures and relative humidity conditions relevant for mixed-phase clouds. We find that at the tested conditions, there is no effect on the ice nucleation ability of the particles due to the organic coating. Furthermore, the two dust samples do not show variability within measurement uncertainty. Particle size and surface area may play a role in any difference observed.
Yvonne Boose, Philipp Baloh, Michael Plötze, Johannes Ofner, Hinrich Grothe, Berko Sierau, Ulrike Lohmann, and Zamin A. Kanji
Atmos. Chem. Phys., 19, 1059–1076, https://doi.org/10.5194/acp-19-1059-2019, https://doi.org/10.5194/acp-19-1059-2019, 2019
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The role non-mineral components play in the freezing behavior of atmospheric desert dust is not well known. In this study, we use chemical imaging methods to investigate this for airborne and surface-collected desert dust samples. We find that in most cases the ice nucleation behavior is determined by the dust mineralogical composition. However, volatile organic material can coat active sites and decrease the dust ice nucleation ability, while biological particles can significantly increase it.
Mikhail Paramonov, Robert O. David, Ruben Kretzschmar, and Zamin A. Kanji
Atmos. Chem. Phys., 18, 16515–16536, https://doi.org/10.5194/acp-18-16515-2018, https://doi.org/10.5194/acp-18-16515-2018, 2018
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The paper presents an overview of the ice nucleation activity of surface-collected mineral and soil dust. Emphasis is placed on disentangling the effects of mineral, biogenic and soluble components of the dust on its ice nucleation activity. The results revealed that it is not possible to predict the ice nucleation activity of the surface-collected dust based on the presence and amount of certain minerals or any particular class of compounds, such as soluble or proteinaceous/organic compounds.
Paul J. DeMott, Ottmar Möhler, Daniel J. Cziczo, Naruki Hiranuma, Markus D. Petters, Sarah S. Petters, Franco Belosi, Heinz G. Bingemer, Sarah D. Brooks, Carsten Budke, Monika Burkert-Kohn, Kristen N. Collier, Anja Danielczok, Oliver Eppers, Laura Felgitsch, Sarvesh Garimella, Hinrich Grothe, Paul Herenz, Thomas C. J. Hill, Kristina Höhler, Zamin A. Kanji, Alexei Kiselev, Thomas Koop, Thomas B. Kristensen, Konstantin Krüger, Gourihar Kulkarni, Ezra J. T. Levin, Benjamin J. Murray, Alessia Nicosia, Daniel O'Sullivan, Andreas Peckhaus, Michael J. Polen, Hannah C. Price, Naama Reicher, Daniel A. Rothenberg, Yinon Rudich, Gianni Santachiara, Thea Schiebel, Jann Schrod, Teresa M. Seifried, Frank Stratmann, Ryan C. Sullivan, Kaitlyn J. Suski, Miklós Szakáll, Hans P. Taylor, Romy Ullrich, Jesus Vergara-Temprado, Robert Wagner, Thomas F. Whale, Daniel Weber, André Welti, Theodore W. Wilson, Martin J. Wolf, and Jake Zenker
Atmos. Meas. Tech., 11, 6231–6257, https://doi.org/10.5194/amt-11-6231-2018, https://doi.org/10.5194/amt-11-6231-2018, 2018
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The ability to measure ice nucleating particles is vital to quantifying their role in affecting clouds and precipitation. Methods for measuring droplet freezing were compared while co-sampling relevant particle types. Measurement correspondence was very good for ice nucleating particles of bacterial and natural soil origin, and somewhat more disparate for those of mineral origin. Results reflect recently improved capabilities and provide direction toward addressing remaining measurement issues.
Fabian Mahrt, Claudia Marcolli, Robert O. David, Philippe Grönquist, Eszter J. Barthazy Meier, Ulrike Lohmann, and Zamin A. Kanji
Atmos. Chem. Phys., 18, 13363–13392, https://doi.org/10.5194/acp-18-13363-2018, https://doi.org/10.5194/acp-18-13363-2018, 2018
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The ice nucleation ability of different soot particles in the cirrus and mixed-phase cloud temperature regime is presented. The impact of aerosol particle size, particle morphology, organic matter and hydrophilicity on ice nucleation is examined. We propose ice nucleation proceeds via a pore condensation freezing mechanism for soot particles with the necessary physicochemical properties that nucleated ice well below water saturation.
Larissa Lacher, Ulrike Lohmann, Yvonne Boose, Assaf Zipori, Erik Herrmann, Nicolas Bukowiecki, Martin Steinbacher, and Zamin A. Kanji
Atmos. Chem. Phys., 17, 15199–15224, https://doi.org/10.5194/acp-17-15199-2017, https://doi.org/10.5194/acp-17-15199-2017, 2017
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We characterize the new Horizontal Ice Nucleation Chamber HINC to measure ambient ice nucleating particle concentrations at mixed‐phase cloud conditions. Results from winter measurements at the High Altitude Research Station Jungfraujoch compare well to previous measurements. We find increased ice nucleating particle concentrations during the influence of Saharan dust events and marine events, which highlights the importance of these species on ice nucleation in the free troposphere.
Monika Burkert-Kohn, Heike Wex, André Welti, Susan Hartmann, Sarah Grawe, Lisa Hellner, Paul Herenz, James D. Atkinson, Frank Stratmann, and Zamin A. Kanji
Atmos. Chem. Phys., 17, 11683–11705, https://doi.org/10.5194/acp-17-11683-2017, https://doi.org/10.5194/acp-17-11683-2017, 2017
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Several instruments can investigate properties of ice-nucleating particles (INPs), which are crucial to understanding ice cloud formation. We intercompare four online ice nucleation counters and reasonable agreement is found when the same ice nucleation mode is tested. A variable scaling factor was necessary to reconcile condensation freezing results with immersion freezing. Factors related to instrumental setup and aerosol generation are discussed to explain observed differences.
Sarvesh Garimella, Daniel A. Rothenberg, Martin J. Wolf, Robert O. David, Zamin A. Kanji, Chien Wang, Michael Rösch, and Daniel J. Cziczo
Atmos. Chem. Phys., 17, 10855–10864, https://doi.org/10.5194/acp-17-10855-2017, https://doi.org/10.5194/acp-17-10855-2017, 2017
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This study investigates systematic and variable low bias in the measurement of ice nucleating particle concentration using continuous flow diffusion chambers. We find that non-ideal instrument behavior exposes particles to different humidities and/or temperatures than predicted from theory. We use a machine learning approach to quantify and minimize the uncertainty associated with this measurement bias.
Yvonne Boose, André Welti, James Atkinson, Fabiola Ramelli, Anja Danielczok, Heinz G. Bingemer, Michael Plötze, Berko Sierau, Zamin A. Kanji, and Ulrike Lohmann
Atmos. Chem. Phys., 16, 15075–15095, https://doi.org/10.5194/acp-16-15075-2016, https://doi.org/10.5194/acp-16-15075-2016, 2016
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We compare the immersion freezing behavior of four airborne to 11 surface-collected dust samples to investigate the role of different minerals for atmospheric ice nucleation on desert dust. We find that present K-feldspars dominate at T > 253 K, while quartz does at colder temperatures, and surface-collected dust samples are not necessarily representative for airborne dust. For improved ice cloud prediction, modeling of quartz and feldspar emission and transport are key.
Yvonne Boose, Berko Sierau, M. Isabel García, Sergio Rodríguez, Andrés Alastuey, Claudia Linke, Martin Schnaiter, Piotr Kupiszewski, Zamin A. Kanji, and Ulrike Lohmann
Atmos. Chem. Phys., 16, 9067–9087, https://doi.org/10.5194/acp-16-9067-2016, https://doi.org/10.5194/acp-16-9067-2016, 2016
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Mineral dust is known to be among the most prevalent ice-nucleating particles (INPs) in the atmosphere, playing a crucial role for ice cloud formation. We present 2 months of ground-based in situ measurements of INP concentrations in the free troposphere close to the largest global dust source, the Sahara. We find that some atmospheric processes such as mixing with biological particles and ammonium increase the dust INP ability. This is important when predicting INPs based on emissions.
N. Hiranuma, S. Augustin-Bauditz, H. Bingemer, C. Budke, J. Curtius, A. Danielczok, K. Diehl, K. Dreischmeier, M. Ebert, F. Frank, N. Hoffmann, K. Kandler, A. Kiselev, T. Koop, T. Leisner, O. Möhler, B. Nillius, A. Peckhaus, D. Rose, S. Weinbruch, H. Wex, Y. Boose, P. J. DeMott, J. D. Hader, T. C. J. Hill, Z. A. Kanji, G. Kulkarni, E. J. T. Levin, C. S. McCluskey, M. Murakami, B. J. Murray, D. Niedermeier, M. D. Petters, D. O'Sullivan, A. Saito, G. P. Schill, T. Tajiri, M. A. Tolbert, A. Welti, T. F. Whale, T. P. Wright, and K. Yamashita
Atmos. Chem. Phys., 15, 2489–2518, https://doi.org/10.5194/acp-15-2489-2015, https://doi.org/10.5194/acp-15-2489-2015, 2015
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Seventeen ice nucleation measurement techniques contributed to investigate the immersion freezing behavior of illite NX. All data showed a similar temperature trend, but the measured ice nucleation activity was on average smaller for the wet suspended samples and higher for the dry-dispersed aerosol samples at high temperatures. A continued investigation and collaboration is necessary to obtain further insights into consistency or diversity of ice nucleation measurements.
H. Wex, S. Augustin-Bauditz, Y. Boose, C. Budke, J. Curtius, K. Diehl, A. Dreyer, F. Frank, S. Hartmann, N. Hiranuma, E. Jantsch, Z. A. Kanji, A. Kiselev, T. Koop, O. Möhler, D. Niedermeier, B. Nillius, M. Rösch, D. Rose, C. Schmidt, I. Steinke, and F. Stratmann
Atmos. Chem. Phys., 15, 1463–1485, https://doi.org/10.5194/acp-15-1463-2015, https://doi.org/10.5194/acp-15-1463-2015, 2015
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Immersion freezing measurements from seven different measurement techniques were intercompared using a biological ice nucleating material from bacteria. Although different techniques examined differently concentrated droplets, it was possible to find a uniform description, which showed that results from all experiments were generally in good agreement and were also in agreement with parameterizations published earlier in literature.
C. Chou, Z. A. Kanji, O. Stetzer, T. Tritscher, R. Chirico, M. F. Heringa, E. Weingartner, A. S. H. Prévôt, U. Baltensperger, and U. Lohmann
Atmos. Chem. Phys., 13, 761–772, https://doi.org/10.5194/acp-13-761-2013, https://doi.org/10.5194/acp-13-761-2013, 2013
Christopher Fuchs, Fabiola Ramelli, Anna J. Miller, Nadja Omanovic, Robert Spirig, Huiying Zhang, Patric Seifert, Kevin Ohneiser, Ulrike Lohmann, and Jan Henneberger
EGUsphere, https://doi.org/10.5194/egusphere-2025-688, https://doi.org/10.5194/egusphere-2025-688, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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We quantify diffusional ice crystal growth in natural clouds using cloud seeding experiments. We report growth rates for 14 experiments between -5.1°C and -8.3°C and observe strong variations depending on the cloud characteristics. Comparing our growth rates to laboratory data, we found similar temperature-dependent trends, but the laboratory rates are higher. This data fills the gap in quantitative in situ observation of ice crystal growth, helping to validate models and laboratory experiments.
Christopher Fuchs, Fabiola Ramelli, David Schweizer, Ulrike Lohmann, and Jan Henneberger
EGUsphere, https://doi.org/10.5194/egusphere-2024-3695, https://doi.org/10.5194/egusphere-2024-3695, 2025
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We present a new instrument based on digital in-line holography (SmHOLIMO) for in situ cloud measurements. SmHOLIMO is designed to specifically measure small cloud droplets with diameters >3.7 μm. This way we retrieve accurate cloud droplet size distributions, which are crucial to understand the evolution and governing microphysical processes of a cloud. Results of a field study are compared to co-located measurements of a second holographic imager, microwave radiometer, and cloud radar.
Judith Kleinheins, Nadia Shardt, Ulrike Lohmann, and Claudia Marcolli
Atmos. Chem. Phys., 25, 881–903, https://doi.org/10.5194/acp-25-881-2025, https://doi.org/10.5194/acp-25-881-2025, 2025
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We model the cloud condensation nuclei (CCN) activation of sea spray aerosol particles with classical Köhler theory and with a new model approach that takes surface tension lowering into account. We categorize organic compounds into weak, intermediate, and strong surfactants, and we outline for which composition surface tension lowering is important. The results suggest that surface tension lowering allows sea spray aerosol particles in the Aitken mode to be a source of CCN in marine updraughts.
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
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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, Golnaz Roudsari, Ana A. Piedehierro, and André Welti
EGUsphere, https://doi.org/10.5194/egusphere-2024-4095, https://doi.org/10.5194/egusphere-2024-4095, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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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.
Nadja Omanovic, Brigitta Goger, and Ulrike Lohmann
Atmos. Chem. Phys., 24, 14145–14175, https://doi.org/10.5194/acp-24-14145-2024, https://doi.org/10.5194/acp-24-14145-2024, 2024
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We evaluated the numerical weather model ICON in two horizontal resolutions with two bulk microphysics schemes over hilly and complex terrain in Switzerland and Austria, respectively. We focused on the model's ability to simulate mid-level clouds in summer and winter. By combining observational data from two different field campaigns, we show that an increase in the horizontal resolution and a more advanced cloud microphysics scheme is strongly beneficial for cloud representation.
Anna J. Miller, Christopher Fuchs, Fabiola Ramelli, Huiying Zhang, Nadja Omanovic, Robert Spirig, Claudia Marcolli, Zamin A. Kanji, Ulrike Lohmann, and Jan Henneberger
EGUsphere, https://doi.org/10.5194/egusphere-2024-3230, https://doi.org/10.5194/egusphere-2024-3230, 2024
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We analyzed the ability of silver iodide particles to form ice crystals in naturally-occurring liquid clouds below 0 °C and found that ≈0.1−1 % of particles nucleate ice, with a negative dependence on temperature. Contextualizing our results with previous laboratory studies, we help to bridge the gap between laboratory and field experiments and which also helps to inform future cloud seeding projects.
Baptiste Testa, Lukas Durdina, Jacinta Edebeli, Curdin Spirig, and Zamin A. Kanji
Atmos. Chem. Phys., 24, 10409–10424, https://doi.org/10.5194/acp-24-10409-2024, https://doi.org/10.5194/acp-24-10409-2024, 2024
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Aviation soot residuals released from contrails can become compacted upon sublimation of the ice crystals, generating new voids in the aggregates where ice nucleation can occur. Here we show that contrail-processed soot is highly compact but that it remains unable to form ice at a relative humidity different from that required for the formation of background cirrus from the more ubiquitous aqueous solution droplets, suggesting that it will not perturb cirrus cloud formation via ice nucleation.
Kai Jeggle, David Neubauer, Hanin Binder, and Ulrike Lohmann
EGUsphere, https://doi.org/10.5194/egusphere-2024-2559, https://doi.org/10.5194/egusphere-2024-2559, 2024
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This work uncovers the formation regimes of cirrus clouds and how dust particles influence their properties. By applying machine learning to a combination of satellite and reanalysis data, cirrus clouds are classified into different formation regimes. Depending on the regime, increasing dust aerosol concentrations can either decrease or increase the number of ice crystals. This challenges the idea of using cloud seeding to cool the planet, as it may unintentionally lead to warming instead.
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.
Nadja Omanovic, Sylvaine Ferrachat, Christopher Fuchs, Jan Henneberger, Anna J. Miller, Kevin Ohneiser, Fabiola Ramelli, Patric Seifert, Robert Spirig, Huiying Zhang, and Ulrike Lohmann
Atmos. Chem. Phys., 24, 6825–6844, https://doi.org/10.5194/acp-24-6825-2024, https://doi.org/10.5194/acp-24-6825-2024, 2024
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We present simulations with a high-resolution numerical weather prediction model to study the growth of ice crystals in low clouds following glaciogenic seeding. We show that the simulated ice crystals grow slower than observed and do not consume as many cloud droplets as measured in the field. This may have implications for forecasting precipitation, as the ice phase is crucial for precipitation at middle and high latitudes.
Ulrike Proske, Sylvaine Ferrachat, and Ulrike Lohmann
Atmos. Chem. Phys., 24, 5907–5933, https://doi.org/10.5194/acp-24-5907-2024, https://doi.org/10.5194/acp-24-5907-2024, 2024
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Climate models include treatment of aerosol particles because these influence clouds and radiation. Over time their representation has grown increasingly detailed. This complexity may hinder our understanding of model behaviour. Thus here we simplify the aerosol representation of our climate model by prescribing mean concentrations, which saves run time and helps to discover unexpected model behaviour. We conclude that simplifications provide a new perspective for model study and development.
Zane Dedekind, Ulrike Proske, Sylvaine Ferrachat, Ulrike Lohmann, and David Neubauer
Atmos. Chem. Phys., 24, 5389–5404, https://doi.org/10.5194/acp-24-5389-2024, https://doi.org/10.5194/acp-24-5389-2024, 2024
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Ice particles precipitating into lower clouds from an upper cloud, the seeder–feeder process, can enhance precipitation. A numerical modeling study conducted in the Swiss Alps found that 48 % of observed clouds were overlapping, with the seeder–feeder process occurring in 10 % of these clouds. Inhibiting the seeder–feeder process reduced the surface precipitation and ice particle growth rates, which were further reduced when additional ice multiplication processes were included in the model.
Baptiste Testa, Lukas Durdina, Peter A. Alpert, Fabian Mahrt, Christopher H. Dreimol, Jacinta Edebeli, Curdin Spirig, Zachary C. J. Decker, Julien Anet, and Zamin A. Kanji
Atmos. Chem. Phys., 24, 4537–4567, https://doi.org/10.5194/acp-24-4537-2024, https://doi.org/10.5194/acp-24-4537-2024, 2024
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Laboratory experiments on the ice nucleation of real commercial aviation soot particles are investigated for their cirrus cloud formation potential. Our results show that aircraft-emitted soot in the upper troposphere will be poor ice-nucleating particles. Measuring the soot particle morphology and modifying their mixing state allow us to elucidate why these particles are ineffective at forming ice, in contrast to previously used soot surrogates.
Anna J. Miller, Fabiola Ramelli, Christopher Fuchs, Nadja Omanovic, Robert Spirig, Huiying Zhang, Ulrike Lohmann, Zamin A. Kanji, and Jan Henneberger
Atmos. Meas. Tech., 17, 601–625, https://doi.org/10.5194/amt-17-601-2024, https://doi.org/10.5194/amt-17-601-2024, 2024
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We present a method for aerosol and cloud research using two uncrewed aerial vehicles (UAVs). The UAVs have a propeller heating mechanism that allows flights in icing conditions, which has so far been a limitation for cloud research with UAVs. One UAV burns seeding flares, producing a plume of particles that causes ice formation in supercooled clouds. The second UAV measures aerosol size distributions and is used for measuring the seeding plume or for characterizing the boundary layer.
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
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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.
Guangyu Li, Elise K. Wilbourn, Zezhen Cheng, Jörg Wieder, Allison Fagerson, Jan Henneberger, Ghislain Motos, Rita Traversi, Sarah D. Brooks, Mauro Mazzola, Swarup China, Athanasios Nenes, Ulrike Lohmann, Naruki Hiranuma, and Zamin A. Kanji
Atmos. Chem. Phys., 23, 10489–10516, https://doi.org/10.5194/acp-23-10489-2023, https://doi.org/10.5194/acp-23-10489-2023, 2023
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In this work, we present results from an Arctic field campaign (NASCENT) in Ny-Ålesund, Svalbard, on the abundance, variability, physicochemical properties, and potential sources of ice-nucleating particles (INPs) relevant for mixed-phase cloud formation. This work improves the data coverage of Arctic INPs and aerosol properties, allowing for the validation of models predicting cloud microphysical and radiative properties of mixed-phase clouds in the rapidly warming Arctic.
Bernhard M. Enz, Jan P. Engelmann, and Ulrike Lohmann
Geosci. Model Dev., 16, 5093–5112, https://doi.org/10.5194/gmd-16-5093-2023, https://doi.org/10.5194/gmd-16-5093-2023, 2023
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An algorithm to track tropical cyclones in model simulation data has been developed. The algorithm uses many combinations of varying parameter thresholds to detect weaker phases of tropical cyclones while still being resilient to false positives. It is shown that the algorithm performs well and adequately represents the tropical cyclone activity of the underlying simulation data. The impact of false positives on overall tropical cyclone activity is shown to be insignificant.
Dimitri Castarède, Zoé Brasseur, Yusheng Wu, Zamin A. Kanji, Markus Hartmann, Lauri Ahonen, Merete Bilde, Markku Kulmala, Tuukka Petäjä, Jan B. C. Pettersson, Berko Sierau, Olaf Stetzer, Frank Stratmann, Birgitta Svenningsson, Erik Swietlicki, Quynh Thu Nguyen, Jonathan Duplissy, and Erik S. Thomson
Atmos. Meas. Tech., 16, 3881–3899, https://doi.org/10.5194/amt-16-3881-2023, https://doi.org/10.5194/amt-16-3881-2023, 2023
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Clouds play a key role in Earth’s climate by influencing the surface energy budget. Certain types of atmospheric aerosols, called ice-nucleating particles (INPs), induce the formation of ice in clouds and, thus, often initiate precipitation formation. The Portable Ice Nucleation Chamber 2 (PINCii) is a new instrument developed to study ice formation and to conduct ambient measurements of INPs, allowing us to investigate the sources and properties of the atmospheric aerosols that can act as INPs.
Colin Tully, David Neubauer, Diego Villanueva, and Ulrike Lohmann
Atmos. Chem. Phys., 23, 7673–7698, https://doi.org/10.5194/acp-23-7673-2023, https://doi.org/10.5194/acp-23-7673-2023, 2023
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This study details the first attempt with a GCM to simulate a fully prognostic aerosol species specifically for cirrus climate intervention. The new approach is in line with the real-world delivery mechanism via aircraft. However, to achieve an appreciable signal from seeding, smaller particles were needed, and their mass emissions needed to be scaled by at least a factor of 100. These biases contributed to either overseeding or small and insignificant effects in response to seeding cirrus.
Joschka Pfeifer, Naser G. A. Mahfouz, Benjamin C. Schulze, Serge Mathot, Dominik Stolzenburg, Rima Baalbaki, Zoé Brasseur, Lucia Caudillo, Lubna Dada, Manuel Granzin, Xu-Cheng He, Houssni Lamkaddam, Brandon Lopez, Vladimir Makhmutov, Ruby Marten, Bernhard Mentler, Tatjana Müller, Antti Onnela, Maxim Philippov, Ana A. Piedehierro, Birte Rörup, Meredith Schervish, Ping Tian, Nsikanabasi S. Umo, Dongyu S. Wang, Mingyi Wang, Stefan K. Weber, André Welti, Yusheng Wu, Marcel Zauner-Wieczorek, Antonio Amorim, Imad El Haddad, Markku Kulmala, Katrianne Lehtipalo, Tuukka Petäjä, António Tomé, Sander Mirme, Hanna E. Manninen, Neil M. Donahue, Richard C. Flagan, Andreas Kürten, Joachim Curtius, and Jasper Kirkby
Atmos. Chem. Phys., 23, 6703–6718, https://doi.org/10.5194/acp-23-6703-2023, https://doi.org/10.5194/acp-23-6703-2023, 2023
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Attachment rate coefficients between ions and charged aerosol particles determine their lifetimes and may also influence cloud dynamics and aerosol processing. Here we present novel experiments that measure ion–aerosol attachment rate coefficients for multiply charged aerosol particles under atmospheric conditions in the CERN CLOUD chamber. Our results provide experimental discrimination between various theoretical models.
Lucía Caudillo, Mihnea Surdu, Brandon Lopez, Mingyi Wang, Markus Thoma, Steffen Bräkling, Angela Buchholz, Mario Simon, Andrea C. Wagner, Tatjana Müller, Manuel Granzin, Martin Heinritzi, Antonio Amorim, David M. Bell, Zoé Brasseur, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Xu-Cheng He, Houssni Lamkaddam, Naser G. A. Mahfouz, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Roy L. Mauldin, Bernhard Mentler, Antti Onnela, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Birte Rörup, Wiebke Scholz, Jiali Shen, Dominik Stolzenburg, Christian Tauber, Ping Tian, António Tomé, Nsikanabasi Silas Umo, Dongyu S. Wang, Yonghong Wang, Stefan K. Weber, André Welti, Marcel Zauner-Wieczorek, Urs Baltensperger, Richard C. Flagan, Armin Hansel, Jasper Kirkby, Markku Kulmala, Katrianne Lehtipalo, Douglas R. Worsnop, Imad El Haddad, Neil M. Donahue, Alexander L. Vogel, Andreas Kürten, and Joachim Curtius
Atmos. Chem. Phys., 23, 6613–6631, https://doi.org/10.5194/acp-23-6613-2023, https://doi.org/10.5194/acp-23-6613-2023, 2023
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In this study, we present an intercomparison of four different techniques for measuring the chemical composition of nanoparticles. The intercomparison was performed based on the observed chemical composition, calculated volatility, and analysis of the thermograms. We found that the methods generally agree on the most important compounds that are found in the nanoparticles. However, they do see different parts of the organic spectrum. We suggest potential explanations for these differences.
Colin Tully, David Neubauer, and Ulrike Lohmann
Geosci. Model Dev., 16, 2957–2973, https://doi.org/10.5194/gmd-16-2957-2023, https://doi.org/10.5194/gmd-16-2957-2023, 2023
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A new method to simulate deterministic ice nucleation processes based on the differential activated fraction was evaluated against a cumulative approach. Box model simulations of heterogeneous-only ice nucleation within cirrus suggest that the latter approach likely underpredicts the ice crystal number concentration. Longer simulations with a GCM show that choosing between these two approaches impacts ice nucleation competition within cirrus but leads to small and insignificant climate effects.
Zane Dedekind, Jacopo Grazioli, Philip H. Austin, and Ulrike Lohmann
Atmos. Chem. Phys., 23, 2345–2364, https://doi.org/10.5194/acp-23-2345-2023, https://doi.org/10.5194/acp-23-2345-2023, 2023
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Simulations allowing ice particles to collide with one another producing more ice particles represented surface observations of ice particles accurately. An increase in ice particles formed through collisions was related to sharp changes in the wind direction and speed with height. Changes in wind speed and direction can therefore cause more enhanced collisions between ice particles and alter how fast and how much precipitation forms. Simulations were conducted with the atmospheric model COSMO.
Fabian Mahrt, Carolin Rösch, Kunfeng Gao, Christopher H. Dreimol, Maria A. Zawadowicz, and Zamin A. Kanji
Atmos. Chem. Phys., 23, 1285–1308, https://doi.org/10.5194/acp-23-1285-2023, https://doi.org/10.5194/acp-23-1285-2023, 2023
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Major aerosol types emitted by biomass burning include soot, ash, and charcoal particles. Here, we investigated the ice nucleation activity of 400 nm size-selected particles of two different pyrolyis-derived charcoal types in the mixed phase and cirrus cloud regime. We find that ice nucleation is constrained to cirrus cloud conditions, takes place via pore condensation and freezing, and is largely governed by the particle porosity and mineral content.
Julie Thérèse Pasquier, Jan Henneberger, Fabiola Ramelli, Annika Lauber, Robert Oscar David, Jörg Wieder, Tim Carlsen, Rosa Gierens, Marion Maturilli, and Ulrike Lohmann
Atmos. Chem. Phys., 22, 15579–15601, https://doi.org/10.5194/acp-22-15579-2022, https://doi.org/10.5194/acp-22-15579-2022, 2022
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It is important to understand how ice crystals and cloud droplets form in clouds, as their concentrations and sizes determine the exact radiative properties of the clouds. Normally, ice crystals form from aerosols, but we found evidence for the formation of additional ice crystals from the original ones over a large temperature range within Arctic clouds. In particular, additional ice crystals were formed during collisions of several ice crystals or during the freezing of large cloud droplets.
Guangyu Li, Jörg Wieder, Julie T. Pasquier, Jan Henneberger, and Zamin A. Kanji
Atmos. Chem. Phys., 22, 14441–14454, https://doi.org/10.5194/acp-22-14441-2022, https://doi.org/10.5194/acp-22-14441-2022, 2022
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The concentration of ice-nucleating particles (INPs) is atmospherically relevant for primary ice formation in clouds. In this work, from 12 weeks of field measurement data in the Arctic, we developed a new parameterization to predict INP concentrations applicable for pristine background conditions based only on temperature. The INP parameterization could improve the cloud microphysical representation in climate models, aiding in Arctic climate predictions.
Florin N. Isenrich, Nadia Shardt, Michael Rösch, Julia Nette, Stavros Stavrakis, Claudia Marcolli, Zamin A. Kanji, Andrew J. deMello, and Ulrike Lohmann
Atmos. Meas. Tech., 15, 5367–5381, https://doi.org/10.5194/amt-15-5367-2022, https://doi.org/10.5194/amt-15-5367-2022, 2022
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Ice nucleation in the atmosphere influences cloud properties and lifetimes. Microfluidic instruments have recently been used to investigate ice nucleation, but these instruments are typically made out of a polymer that contributes to droplet instability over extended timescales and relatively high temperature uncertainty. To address these drawbacks, we develop and validate a new microfluidic instrument that uses fluoropolymer tubing to extend droplet stability and improve temperature accuracy.
Colin Tully, David Neubauer, Nadja Omanovic, and Ulrike Lohmann
Atmos. Chem. Phys., 22, 11455–11484, https://doi.org/10.5194/acp-22-11455-2022, https://doi.org/10.5194/acp-22-11455-2022, 2022
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The proposed geoengineering method, cirrus cloud thinning, was evaluated using a more physically based microphysics scheme coupled to a more realistic approach for calculating ice cloud fractions in the ECHAM-HAM GCM. Sensitivity tests reveal that using the new ice cloud fraction approach and increasing the critical ice saturation ratio for ice nucleation on seeding particles reduces warming from overseeding. However, this geoengineering method is unlikely to be feasible on a global scale.
Jörg Wieder, Nikola Ihn, Claudia Mignani, Moritz Haarig, Johannes Bühl, Patric Seifert, Ronny Engelmann, Fabiola Ramelli, Zamin A. Kanji, Ulrike Lohmann, and Jan Henneberger
Atmos. Chem. Phys., 22, 9767–9797, https://doi.org/10.5194/acp-22-9767-2022, https://doi.org/10.5194/acp-22-9767-2022, 2022
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Ice formation and its evolution in mixed-phase clouds are still uncertain. We evaluate the lidar retrieval of ice-nucleating particle concentration in dust-dominated and continental air masses over the Swiss Alps with in situ observations. A calibration factor to improve the retrieval from continental air masses is proposed. Ice multiplication factors are obtained with a new method utilizing remote sensing. Our results indicate that secondary ice production occurs at temperatures down to −30 °C.
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
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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.
Cyril Brunner, Benjamin T. Brem, Martine Collaud Coen, Franz Conen, Martin Steinbacher, Martin Gysel-Beer, and Zamin A. Kanji
Atmos. Chem. Phys., 22, 7557–7573, https://doi.org/10.5194/acp-22-7557-2022, https://doi.org/10.5194/acp-22-7557-2022, 2022
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Microscopic particles called ice-nucleating particles (INPs) are essential for ice crystals to form in clouds. INPs are a tiny proportion of atmospheric aerosol, and their abundance is poorly constrained. We study how the concentration of INPs changes diurnally and seasonally at a mountaintop station in central Europe. Unsurprisingly, a diurnal cycle is only found when considering air masses that have had lower-altitude ground contact. The highest INP concentrations occur in spring.
Cuiqi Zhang, Zhijun Wu, Jingchuan Chen, Jie Chen, Lizi Tang, Wenfei Zhu, Xiangyu Pei, Shiyi Chen, Ping Tian, Song Guo, Limin Zeng, Min Hu, and Zamin A. Kanji
Atmos. Chem. Phys., 22, 7539–7556, https://doi.org/10.5194/acp-22-7539-2022, https://doi.org/10.5194/acp-22-7539-2022, 2022
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The immersion ice nucleation effectiveness of aerosols from multiple sources in the urban environment remains elusive. In this study, we demonstrate that the immersion ice-nucleating particle (INP) concentration increased dramatically during a dust event in an urban atmosphere. Pollutant aerosols, including inorganic salts formed through secondary transformation (SIA) and black carbon (BC), might not act as effective INPs under mixed-phase cloud conditions.
Kunfeng Gao, Chong-Wen Zhou, Eszter J. Barthazy Meier, and Zamin A. Kanji
Atmos. Chem. Phys., 22, 5331–5364, https://doi.org/10.5194/acp-22-5331-2022, https://doi.org/10.5194/acp-22-5331-2022, 2022
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Incomplete combustion of fossil fuel produces carbonaceous particles called soot. These particles can affect cloud formation by acting as centres for droplet or ice formation. The atmospheric residence time of soot particles is of the order of days to weeks, which can result in them becoming coated by various trace species in the atmosphere such as acids. In this study, we quantify the cirrus cloud-forming ability of soot particles coated with the atmospherically ubiquitous sulfuric acid.
Zoé Brasseur, Dimitri Castarède, Erik S. Thomson, Michael P. Adams, Saskia Drossaart van Dusseldorp, Paavo Heikkilä, Kimmo Korhonen, Janne Lampilahti, Mikhail Paramonov, Julia Schneider, Franziska Vogel, Yusheng Wu, Jonathan P. D. Abbatt, Nina S. Atanasova, Dennis H. Bamford, Barbara Bertozzi, Matthew Boyer, David Brus, Martin I. Daily, Romy Fösig, Ellen Gute, Alexander D. Harrison, Paula Hietala, Kristina Höhler, Zamin A. Kanji, Jorma Keskinen, Larissa Lacher, Markus Lampimäki, Janne Levula, Antti Manninen, Jens Nadolny, Maija Peltola, Grace C. E. Porter, Pyry Poutanen, Ulrike Proske, Tobias Schorr, Nsikanabasi Silas Umo, János Stenszky, Annele Virtanen, Dmitri Moisseev, Markku Kulmala, Benjamin J. Murray, Tuukka Petäjä, Ottmar Möhler, and Jonathan Duplissy
Atmos. Chem. Phys., 22, 5117–5145, https://doi.org/10.5194/acp-22-5117-2022, https://doi.org/10.5194/acp-22-5117-2022, 2022
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The present measurement report introduces the ice nucleation campaign organized in Hyytiälä, Finland, in 2018 (HyICE-2018). We provide an overview of the campaign settings, and we describe the measurement infrastructure and operating procedures used. In addition, we use results from ice nucleation instrument inter-comparison to show that the suite of these instruments deployed during the campaign reports consistent results.
Kunfeng Gao, Franz Friebel, Chong-Wen Zhou, and Zamin A. Kanji
Atmos. Chem. Phys., 22, 4985–5016, https://doi.org/10.5194/acp-22-4985-2022, https://doi.org/10.5194/acp-22-4985-2022, 2022
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Soot particles impact cloud formation and radiative properties in the upper atmosphere where aircraft emit carbonaceous particles. We use cloud chambers to mimic the upper atmosphere temperature and humidity to test the influence of the morphology of the soot particles on ice cloud formation. For particles larger than 200 nm, the compacted (densified) samples have a higher affinity for ice crystal formation in the cirrus regime than the fluffy (un-compacted) soot particles of the same sample.
Ulrike Proske, Sylvaine Ferrachat, David Neubauer, Martin Staab, and Ulrike Lohmann
Atmos. Chem. Phys., 22, 4737–4762, https://doi.org/10.5194/acp-22-4737-2022, https://doi.org/10.5194/acp-22-4737-2022, 2022
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Cloud microphysical processes shape cloud properties and are therefore important to represent in climate models. Their parameterization has grown more complex, making the model results more difficult to interpret. Using sensitivity analysis we test how the global aerosol–climate model ECHAM-HAM reacts to changes to these parameterizations. The model is sensitive to the parameterization of ice crystal autoconversion but not to, e.g., self-collection, suggesting that it may be simplified.
Jörg Wieder, Claudia Mignani, Mario Schär, Lucie Roth, Michael Sprenger, Jan Henneberger, Ulrike Lohmann, Cyril Brunner, and Zamin A. Kanji
Atmos. Chem. Phys., 22, 3111–3130, https://doi.org/10.5194/acp-22-3111-2022, https://doi.org/10.5194/acp-22-3111-2022, 2022
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We investigate the variation in ice-nucleating particles (INPs) relevant for primary ice formation in mixed-phased clouds over the Alps based on simultaneous in situ observations at a mountaintop and a nearby high valley (1060 m height difference). In most cases, advection from the surrounding lower regions was responsible for changes in INP concentration, causing a diurnal cycle at the mountaintop. Our study underlines the importance of the planetary boundary layer as an INP reserve.
Cyril Brunner, Benjamin T. Brem, Martine Collaud Coen, Franz Conen, Maxime Hervo, Stephan Henne, Martin Steinbacher, Martin Gysel-Beer, and Zamin A. Kanji
Atmos. Chem. Phys., 21, 18029–18053, https://doi.org/10.5194/acp-21-18029-2021, https://doi.org/10.5194/acp-21-18029-2021, 2021
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Special microscopic particles called ice-nucleating particles (INPs) are essential for ice crystals to form in the atmosphere. INPs are sparse and their atmospheric concentration and properties are not well understood. Mineral dust particles make up a significant fraction of INPs but how much remains unknown. Here, we address this knowledge gap by studying periods when mineral particles are present in large quantities at a mountaintop station in central Europe.
Lucía Caudillo, Birte Rörup, Martin Heinritzi, Guillaume Marie, Mario Simon, Andrea C. Wagner, Tatjana Müller, Manuel Granzin, Antonio Amorim, Farnoush Ataei, Rima Baalbaki, Barbara Bertozzi, Zoé Brasseur, Randall Chiu, Biwu Chu, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Loïc Gonzalez Carracedo, Xu-Cheng He, Victoria Hofbauer, Weimeng Kong, Houssni Lamkaddam, Chuan P. Lee, Brandon Lopez, Naser G. A. Mahfouz, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Dario Massabò, Roy L. Mauldin, Bernhard Mentler, Ugo Molteni, Antti Onnela, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Meredith Schervish, Wiebke Scholz, Benjamin Schulze, Jiali Shen, Dominik Stolzenburg, Yuri Stozhkov, Mihnea Surdu, Christian Tauber, Yee Jun Tham, Ping Tian, António Tomé, Steffen Vogt, Mingyi Wang, Dongyu S. Wang, Stefan K. Weber, André Welti, Wang Yonghong, Wu Yusheng, Marcel Zauner-Wieczorek, Urs Baltensperger, Imad El Haddad, Richard C. Flagan, Armin Hansel, Kristina Höhler, Jasper Kirkby, Markku Kulmala, Katrianne Lehtipalo, Ottmar Möhler, Harald Saathoff, Rainer Volkamer, Paul M. Winkler, Neil M. Donahue, Andreas Kürten, and Joachim Curtius
Atmos. Chem. Phys., 21, 17099–17114, https://doi.org/10.5194/acp-21-17099-2021, https://doi.org/10.5194/acp-21-17099-2021, 2021
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We performed experiments in the CLOUD chamber at CERN at low temperatures to simulate new particle formation in the upper free troposphere (at −30 ºC and −50 ºC). We measured the particle and gas phase and found that most of the compounds present in the gas phase are detected as well in the particle phase. The major compounds in the particles are C8–10 and C18–20. Specifically, we showed that C5 and C15 compounds are detected in a mixed system with isoprene and α-pinene at −30 ºC, 20 % RH.
Larissa Lacher, Hans-Christian Clemen, Xiaoli Shen, Stephan Mertes, Martin Gysel-Beer, Alireza Moallemi, Martin Steinbacher, Stephan Henne, Harald Saathoff, Ottmar Möhler, Kristina Höhler, Thea Schiebel, Daniel Weber, Jann Schrod, Johannes Schneider, and Zamin A. Kanji
Atmos. Chem. Phys., 21, 16925–16953, https://doi.org/10.5194/acp-21-16925-2021, https://doi.org/10.5194/acp-21-16925-2021, 2021
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We investigate ice-nucleating particle properties at Jungfraujoch during the 2017 joint INUIT/CLACE field campaign, to improve the knowledge about those rare particles in a cloud-relevant environment. By quantifying ice-nucleating particles in parallel to single-particle mass spectrometry measurements, we find that mineral dust and aged sea spray particles are potential candidates for ice-nucleating particles. Our findings are supported by ice residual analysis and source region modeling.
Zane Dedekind, Annika Lauber, Sylvaine Ferrachat, and Ulrike Lohmann
Atmos. Chem. Phys., 21, 15115–15134, https://doi.org/10.5194/acp-21-15115-2021, https://doi.org/10.5194/acp-21-15115-2021, 2021
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The RACLETS campaign combined cloud and snow research to improve the understanding of precipitation formation in clouds. A numerical weather prediction model, COSMO, was used to assess the importance of ice crystal enhancement by ice–ice collisions for cloud properties. We found that the number of ice crystals increased by 1 to 3 orders of magnitude when ice–ice collisions were permitted to occur, reducing localized regions of high precipitation and, thereby, improving the model performance.
Paolo Pelucchi, David Neubauer, and Ulrike Lohmann
Geosci. Model Dev., 14, 5413–5434, https://doi.org/10.5194/gmd-14-5413-2021, https://doi.org/10.5194/gmd-14-5413-2021, 2021
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Stratocumulus are thin clouds whose cloud cover is underestimated in climate models partly due to overly low vertical resolution. We develop a scheme that locally refines the vertical grid based on a physical constraint for the cloud top. Global simulations show that the scheme, implemented only in the radiation routine, can increase stratocumulus cloud cover. However, this effect is poorly propagated to the simulated cloud cover. The scheme's limitations and possible ways forward are discussed.
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
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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
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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.
Paraskevi Georgakaki, Aikaterini Bougiatioti, Jörg Wieder, Claudia Mignani, Fabiola Ramelli, Zamin A. Kanji, Jan Henneberger, Maxime Hervo, Alexis Berne, Ulrike Lohmann, and Athanasios Nenes
Atmos. Chem. Phys., 21, 10993–11012, https://doi.org/10.5194/acp-21-10993-2021, https://doi.org/10.5194/acp-21-10993-2021, 2021
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Aerosol and cloud observations coupled with a droplet activation parameterization was used to investigate the aerosol–cloud droplet link in alpine mixed-phase clouds. Predicted droplet number, Nd, agrees with observations and never exceeds a characteristic “limiting droplet number”, Ndlim, which depends solely on σw. Nd becomes velocity limited when it is within 50 % of Ndlim. Identifying when dynamical changes control Nd variability is central for understanding aerosol–cloud interactions.
Fabiola Ramelli, Jan Henneberger, Robert O. David, Johannes Bühl, Martin Radenz, Patric Seifert, Jörg Wieder, Annika Lauber, Julie T. Pasquier, Ronny Engelmann, Claudia Mignani, Maxime Hervo, and Ulrike Lohmann
Atmos. Chem. Phys., 21, 6681–6706, https://doi.org/10.5194/acp-21-6681-2021, https://doi.org/10.5194/acp-21-6681-2021, 2021
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Orographic mixed-phase clouds are an important source of precipitation, but the ice formation processes within them remain uncertain. Here we investigate the origin of ice crystals in a mixed-phase cloud in the Swiss Alps using aerosol and cloud data from in situ and remote sensing observations. We found that ice formation primarily occurs in cloud top generating cells. Our results indicate that secondary ice processes are active in the feeder region, which can enhance orographic precipitation.
Fabiola Ramelli, Jan Henneberger, Robert O. David, Annika Lauber, Julie T. Pasquier, Jörg Wieder, Johannes Bühl, Patric Seifert, Ronny Engelmann, Maxime Hervo, and Ulrike Lohmann
Atmos. Chem. Phys., 21, 5151–5172, https://doi.org/10.5194/acp-21-5151-2021, https://doi.org/10.5194/acp-21-5151-2021, 2021
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Interactions between dynamics, microphysics and orography can enhance precipitation. Yet the exact role of these interactions is still uncertain. Here we investigate the role of low-level blocking and turbulence for precipitation by combining remote sensing and in situ observations. The observations show that blocked flow can induce the formation of feeder clouds and that turbulence can enhance hydrometeor growth, demonstrating the importance of local flow effects for orographic precipitation.
Ulrike Proske, Verena Bessenbacher, Zane Dedekind, Ulrike Lohmann, and David Neubauer
Atmos. Chem. Phys., 21, 5195–5216, https://doi.org/10.5194/acp-21-5195-2021, https://doi.org/10.5194/acp-21-5195-2021, 2021
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Ice crystals falling out of one cloud can initiate freezing in a second cloud below. We estimate the occurrence frequency of this natural cloud seeding over Switzerland from satellite data and sublimation calculations. We find that such situations with an ice cloud above another cloud are frequent and that the falling crystals survive the fall between two clouds in a significant number of cases, suggesting that natural cloud seeding is an important phenomenon over Switzerland.
Annika Lauber, Jan Henneberger, Claudia Mignani, Fabiola Ramelli, Julie T. Pasquier, Jörg Wieder, Maxime Hervo, and Ulrike Lohmann
Atmos. Chem. Phys., 21, 3855–3870, https://doi.org/10.5194/acp-21-3855-2021, https://doi.org/10.5194/acp-21-3855-2021, 2021
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An accurate prediction of the ice crystal number concentration (ICNC) is important to determine the radiation budget, lifetime, and precipitation formation of clouds. Even though secondary-ice processes can increase the ICNC by several orders of magnitude, they are poorly constrained and lack a well-founded quantification. During measurements on a mountain slope, a high ICNC of small ice crystals was observed just below 0 °C, attributed to a secondary-ice process and parametrized in this study.
Claudia Mignani, Jörg Wieder, Michael A. Sprenger, Zamin A. Kanji, Jan Henneberger, Christine Alewell, and Franz Conen
Atmos. Chem. Phys., 21, 657–664, https://doi.org/10.5194/acp-21-657-2021, https://doi.org/10.5194/acp-21-657-2021, 2021
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Most precipitation above land starts with ice in clouds. It is promoted by extremely rare particles. Some ice-nucleating particles (INPs) cause cloud droplets to already freeze above −15°C, a temperature at which many clouds begin to snow. We found that the abundance of such INPs among other particles of similar size is highest in precipitating air masses and lowest when air carries desert dust. This brings us closer to understanding the interactions between land, clouds, and precipitation.
Cyril Brunner and Zamin A. Kanji
Atmos. Meas. Tech., 14, 269–293, https://doi.org/10.5194/amt-14-269-2021, https://doi.org/10.5194/amt-14-269-2021, 2021
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Subvisual microscopic particles in the atmosphere are needed to act as seeds for cloud droplets or ice crystals to form. The microscopic particles, called ice-nucleating particles (INPs), form ice crystals and are rare, and their properties are not well understood, in part because measuring them is challenging and time consuming, and to date has not been automated. Here, we present the first online instrument that can continuously and autonomously measure INP concentration at 243 K.
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.
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
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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.
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
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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
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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.
Robert J. Allen, Steven Turnock, Pierre Nabat, David Neubauer, Ulrike Lohmann, Dirk Olivié, Naga Oshima, Martine Michou, Tongwen Wu, Jie Zhang, Toshihiko Takemura, Michael Schulz, Kostas Tsigaridis, Susanne E. Bauer, Louisa Emmons, Larry Horowitz, Vaishali Naik, Twan van Noije, Tommi Bergman, Jean-Francois Lamarque, Prodromos Zanis, Ina Tegen, Daniel M. Westervelt, Philippe Le Sager, Peter Good, Sungbo Shim, Fiona O'Connor, Dimitris Akritidis, Aristeidis K. Georgoulias, Makoto Deushi, Lori T. Sentman, Jasmin G. John, Shinichiro Fujimori, and William J. Collins
Atmos. Chem. Phys., 20, 9641–9663, https://doi.org/10.5194/acp-20-9641-2020, https://doi.org/10.5194/acp-20-9641-2020, 2020
Robert O. David, Jonas Fahrni, Claudia Marcolli, Fabian Mahrt, Dominik Brühwiler, and Zamin A. Kanji
Atmos. Chem. Phys., 20, 9419–9440, https://doi.org/10.5194/acp-20-9419-2020, https://doi.org/10.5194/acp-20-9419-2020, 2020
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Ice crystal formation plays an important role in controlling the Earth's climate. However, the mechanisms responsible for ice formation in the atmosphere are still uncertain. Here we use surrogates for atmospherically relevant porous particles to determine the role of pore diameter and wettability on the ability of porous particles to nucleate ice in the atmosphere. Our results are consistent with the pore condensation and freeing mechanism.
Mikhail Paramonov, Saskia Drossaart van Dusseldorp, Ellen Gute, Jonathan P. D. Abbatt, Paavo Heikkilä, Jorma Keskinen, Xuemeng Chen, Krista Luoma, Liine Heikkinen, Liqing Hao, Tuukka Petäjä, and Zamin A. Kanji
Atmos. Chem. Phys., 20, 6687–6706, https://doi.org/10.5194/acp-20-6687-2020, https://doi.org/10.5194/acp-20-6687-2020, 2020
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Ice-nucleating particle (INP) measurements were performed in the boreal environment of southern Finland in the winter–spring of 2018. It was found that no single parameter could be used to predict the INP number concentration at the measurement location during the examined time period. It was also not possible to identify physical and chemical properties of ambient INPs despite the complexity of the instrumental set-up. Therefore, this paper addresses the necessity for future INP measurements.
Mattia Righi, Johannes Hendricks, Ulrike Lohmann, Christof Gerhard Beer, Valerian Hahn, Bernd Heinold, Romy Heller, Martina Krämer, Michael Ponater, Christian Rolf, Ina Tegen, and Christiane Voigt
Geosci. Model Dev., 13, 1635–1661, https://doi.org/10.5194/gmd-13-1635-2020, https://doi.org/10.5194/gmd-13-1635-2020, 2020
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A new cloud microphysical scheme is implemented in the global EMAC-MADE3 aerosol model and evaluated. The new scheme features a detailed parameterization for aerosol-driven ice formation in cirrus clouds, accounting for the competition between homogeneous and heterogeneous ice formation processes. The comparison against satellite data and in situ measurements shows that the model performance is in line with similar global coupled models featuring ice cloud parameterizations.
Fabiola Ramelli, Alexander Beck, Jan Henneberger, and Ulrike Lohmann
Atmos. Meas. Tech., 13, 925–939, https://doi.org/10.5194/amt-13-925-2020, https://doi.org/10.5194/amt-13-925-2020, 2020
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Boundary layer clouds are influenced by many physical and dynamical processes, making accurate forecasting difficult. Here we present a new measurement platform on a tethered balloon to measure cloud microphysical and meteorological profiles. The unique combination of holography and balloon-borne observations allows high-resolution measurements in a well-defined volume. Field measurements in stratus clouds over the Swiss Plateau revealed unique microphysical signatures in the cloud structure.
Giulia Saponaro, Moa K. Sporre, David Neubauer, Harri Kokkola, Pekka Kolmonen, Larisa Sogacheva, Antti Arola, Gerrit de Leeuw, Inger H. H. Karset, Ari Laaksonen, and Ulrike Lohmann
Atmos. Chem. Phys., 20, 1607–1626, https://doi.org/10.5194/acp-20-1607-2020, https://doi.org/10.5194/acp-20-1607-2020, 2020
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The understanding of cloud processes is based on the quality of the representation of cloud properties. We compared cloud parameters from three models with satellite observations. We report on the performance of each data source, highlighting strengths and deficiencies, which should be considered when deriving the effect of aerosols on cloud properties.
Robert O. David, Maria Cascajo-Castresana, Killian P. Brennan, Michael Rösch, Nora Els, Julia Werz, Vera Weichlinger, Lin S. Boynton, Sophie Bogler, Nadine Borduas-Dedekind, Claudia Marcolli, and Zamin A. Kanji
Atmos. Meas. Tech., 12, 6865–6888, https://doi.org/10.5194/amt-12-6865-2019, https://doi.org/10.5194/amt-12-6865-2019, 2019
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Here we present the development and applicability of the DRoplet Ice Nuclei Counter Zurich (DRINCZ). DRINCZ allows for ice nuclei in the immersion mode to be quantified between 0 and -25 °C with an uncertainty of ±0.9 °C. Furthermore, we present a new method for assessing biases in drop-freezing apparatuses and cumulative ice-nucleating-particle concentrations from snow samples collected in the Austrian Alps at the Sonnblick Observatory.
Franz Friebel, Prem Lobo, David Neubauer, Ulrike Lohmann, Saskia Drossaart van Dusseldorp, Evelyn Mühlhofer, and Amewu A. Mensah
Atmos. Chem. Phys., 19, 15545–15567, https://doi.org/10.5194/acp-19-15545-2019, https://doi.org/10.5194/acp-19-15545-2019, 2019
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We investigated the change in cloud droplet activity of size-selected soot particles after being exposed to atmospheric levels of ozone over the course of 12 h. For this, we operated a 3 m3 aerosol chamber in continuous-flow mode. The results were fed into a climate model (ECHAM-HAM). We found that the oxidation of soot particles with ozone is a significant source of cloud condensation nuclei in the atmosphere.
Albert Ansmann, Rodanthi-Elisavet Mamouri, Johannes Bühl, Patric Seifert, Ronny Engelmann, Julian Hofer, Argyro Nisantzi, James D. Atkinson, Zamin A. Kanji, Berko Sierau, Mihalis Vrekoussis, and Jean Sciare
Atmos. Chem. Phys., 19, 15087–15115, https://doi.org/10.5194/acp-19-15087-2019, https://doi.org/10.5194/acp-19-15087-2019, 2019
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For the first time, a closure study of the relationship between the ice-nucleating particle concentration (INPC) and ice crystal number concentration (ICNC) in altocumulus and cirrus layers, solely based on ground-based active remote sensing, is presented. The closure studies were conducted in Cyprus. A focus was on altocumulus and cirrus layers which developed in pronounced Saharan dust layers. The closure studies show that heterogeneous ice nucleation can play a dominant role in ice formation.
Simonas Kecorius, Teresa Vogl, Pauli Paasonen, Janne Lampilahti, Daniel Rothenberg, Heike Wex, Sebastian Zeppenfeld, Manuela van Pinxteren, Markus Hartmann, Silvia Henning, Xianda Gong, Andre Welti, Markku Kulmala, Frank Stratmann, Hartmut Herrmann, and Alfred Wiedensohler
Atmos. Chem. Phys., 19, 14339–14364, https://doi.org/10.5194/acp-19-14339-2019, https://doi.org/10.5194/acp-19-14339-2019, 2019
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Arctic sea-ice retreat, atmospheric new particle formation (NPF), and aerosol–cloud interaction may all be linked via a positive feedback mechanism. Understanding the sources of cloud condensation nuclei (CCN) is an important piece in the Arctic amplification puzzle. We show that Arctic newly formed particles do not have to grow beyond the Aitken mode to act as CCN. This is important, because NPF occurrence in the Arctic is expected to increase, making it a significant contributor to CCN budget.
Anina Gilgen, Stiig Wilkenskjeld, Jed O. Kaplan, Thomas Kühn, and Ulrike Lohmann
Clim. Past, 15, 1885–1911, https://doi.org/10.5194/cp-15-1885-2019, https://doi.org/10.5194/cp-15-1885-2019, 2019
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Using the global aerosol–climate model ECHAM-HAM-SALSA, the effect of humans on European climate in the Roman Empire was quantified. Both land use and novel estimates of anthropogenic aerosol emissions were considered. We conducted simulations with fixed sea-surface temperatures to gain a first impression about the anthropogenic impact. While land use effects induced a regional warming for one of the reconstructions, aerosol emissions led to a cooling associated with aerosol–cloud interactions.
Nadine Borduas-Dedekind, Rachele Ossola, Robert O. David, Lin S. Boynton, Vera Weichlinger, Zamin A. Kanji, and Kristopher McNeill
Atmos. Chem. Phys., 19, 12397–12412, https://doi.org/10.5194/acp-19-12397-2019, https://doi.org/10.5194/acp-19-12397-2019, 2019
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During atmospheric transport, dissolved organic matter (DOM) within aqueous aerosols undergoes photochemistry. We find that photochemical processing of DOM increases its ability to form cloud droplets but decreases its ability to form ice crystals over a simulated 4.6 days in the atmosphere. A photomineralization mechanism involving the loss of organic carbon and the production of organic acids, CO and CO2 explains the observed changes and affects the liquid-water-to-ice ratio in clouds.
André Welti, Ulrike Lohmann, and Zamin A. Kanji
Atmos. Chem. Phys., 19, 10901–10918, https://doi.org/10.5194/acp-19-10901-2019, https://doi.org/10.5194/acp-19-10901-2019, 2019
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The ice nucleation ability of singly immersed feldspar particles in suspended water droplets relevant for ice crystal formation under mixed-phase cloud conditions is presented. The effects of particle size, crystal structure, trace metal and mineralogical composition are discussed by testing up to five different diameters in the submicron range and nine different feldspar samples at conditions relevant for ice nucleation in mixed-phase clouds.
David Neubauer, Sylvaine Ferrachat, Colombe Siegenthaler-Le Drian, Philip Stier, Daniel G. Partridge, Ina Tegen, Isabelle Bey, Tanja Stanelle, Harri Kokkola, and Ulrike Lohmann
Geosci. Model Dev., 12, 3609–3639, https://doi.org/10.5194/gmd-12-3609-2019, https://doi.org/10.5194/gmd-12-3609-2019, 2019
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The global aerosol–climate model ECHAM6.3–HAM2.3 as well as the previous model versions ECHAM5.5–HAM2.0 and ECHAM6.1–HAM2.2 are evaluated. The simulation of clouds has improved in ECHAM6.3–HAM2.3. This has an impact on effective radiative forcing due to aerosol–radiation and aerosol–cloud interactions and equilibrium climate sensitivity, which are weaker in ECHAM6.3–HAM2.3 than in the previous model versions.
Gesa K. Eirund, Anna Possner, and Ulrike Lohmann
Atmos. Chem. Phys., 19, 9847–9864, https://doi.org/10.5194/acp-19-9847-2019, https://doi.org/10.5194/acp-19-9847-2019, 2019
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Low-level mixed-phase cloud (MPC) properties can be highly affected by the ambient aerosol concentration, especially in pristine environments like the Arctic. By employing high-resolution model simulations we investigate the response of a MPC over an open ocean and a sea ice surface to aerosol perturbations. While we find a strong initial sensitivity to changes in aerosol concentration in both cloud regimes, the magnitude as well as the long-term cloud response depends on the surface condition.
Remo Dietlicher, David Neubauer, and Ulrike Lohmann
Atmos. Chem. Phys., 19, 9061–9080, https://doi.org/10.5194/acp-19-9061-2019, https://doi.org/10.5194/acp-19-9061-2019, 2019
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Ice crystals in clouds cover a spectrum of shapes and sizes. We show the first results of a consistent representation of the cloud ice spectrum in the climate model ECHAM6-HAM2. The simulated cloud fields are linked to their sources by new diagnostics. We find that only a small fraction of ice clouds is initiated by freezing of cloud droplets in the mixed-phase temperature regime while most ice forms at temperatures colder than −35 °C.
George S. Fanourgakis, Maria Kanakidou, Athanasios Nenes, Susanne E. Bauer, Tommi Bergman, Ken S. Carslaw, Alf Grini, Douglas S. Hamilton, Jill S. Johnson, Vlassis A. Karydis, Alf Kirkevåg, John K. Kodros, Ulrike Lohmann, Gan Luo, Risto Makkonen, Hitoshi Matsui, David Neubauer, Jeffrey R. Pierce, Julia Schmale, Philip Stier, Kostas Tsigaridis, Twan van Noije, Hailong Wang, Duncan Watson-Parris, Daniel M. Westervelt, Yang Yang, Masaru Yoshioka, Nikos Daskalakis, Stefano Decesari, Martin Gysel-Beer, Nikos Kalivitis, Xiaohong Liu, Natalie M. Mahowald, Stelios Myriokefalitakis, Roland Schrödner, Maria Sfakianaki, Alexandra P. Tsimpidi, Mingxuan Wu, and Fangqun Yu
Atmos. Chem. Phys., 19, 8591–8617, https://doi.org/10.5194/acp-19-8591-2019, https://doi.org/10.5194/acp-19-8591-2019, 2019
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Effects of aerosols on clouds are important for climate studies but are among the largest uncertainties in climate projections. This study evaluates the skill of global models to simulate aerosol, cloud condensation nuclei (CCN) and cloud droplet number concentrations (CDNCs). Model results show reduced spread in CDNC compared to CCN due to the negative correlation between the sensitivities of CDNC to aerosol number concentration (air pollution) and updraft velocity (atmospheric dynamics).
Fabian Mahrt, Jörg Wieder, Remo Dietlicher, Helen R. Smith, Chris Stopford, and Zamin A. Kanji
Atmos. Meas. Tech., 12, 3183–3208, https://doi.org/10.5194/amt-12-3183-2019, https://doi.org/10.5194/amt-12-3183-2019, 2019
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A new instrument, the High Speed Particle Phase Discriminator (PPD-HS), is presented, with the goal of quantifying liquid and ice fraction in conditions relevant for mixed-phase clouds. PPD-HS captures the near-forward spatial intensity distribution of scattered light on a single particle basis. Symmetry analysis of the scattering pattern is used to determine the shape of the particles, with cloud droplets and ice crystals producing symmetrical and asymmetrical scattering patterns, respectively.
Stephanie Fiedler, Stefan Kinne, Wan Ting Katty Huang, Petri Räisänen, Declan O'Donnell, Nicolas Bellouin, Philip Stier, Joonas Merikanto, Twan van Noije, Risto Makkonen, and Ulrike Lohmann
Atmos. Chem. Phys., 19, 6821–6841, https://doi.org/10.5194/acp-19-6821-2019, https://doi.org/10.5194/acp-19-6821-2019, 2019
Ina Tegen, David Neubauer, Sylvaine Ferrachat, Colombe Siegenthaler-Le Drian, Isabelle Bey, Nick Schutgens, Philip Stier, Duncan Watson-Parris, Tanja Stanelle, Hauke Schmidt, Sebastian Rast, Harri Kokkola, Martin Schultz, Sabine Schroeder, Nikos Daskalakis, Stefan Barthel, Bernd Heinold, and Ulrike Lohmann
Geosci. Model Dev., 12, 1643–1677, https://doi.org/10.5194/gmd-12-1643-2019, https://doi.org/10.5194/gmd-12-1643-2019, 2019
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We describe a new version of the aerosol–climate model ECHAM–HAM and show tests of the model performance by comparing different aspects of the aerosol distribution with different datasets. The updated version of HAM contains improved descriptions of aerosol processes, including updated emission fields and cloud processes. While there are regional deviations between the model and observations, the model performs well overall.
Zamin A. Kanji, Ryan C. Sullivan, Monika Niemand, Paul J. DeMott, Anthony J. Prenni, Cédric Chou, Harald Saathoff, and Ottmar Möhler
Atmos. Chem. Phys., 19, 5091–5110, https://doi.org/10.5194/acp-19-5091-2019, https://doi.org/10.5194/acp-19-5091-2019, 2019
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The ice nucleation ability of two natural desert dusts coated with a proxy of secondary organic aerosol is presented for temperatures and relative humidity conditions relevant for mixed-phase clouds. We find that at the tested conditions, there is no effect on the ice nucleation ability of the particles due to the organic coating. Furthermore, the two dust samples do not show variability within measurement uncertainty. Particle size and surface area may play a role in any difference observed.
Yvonne Boose, Philipp Baloh, Michael Plötze, Johannes Ofner, Hinrich Grothe, Berko Sierau, Ulrike Lohmann, and Zamin A. Kanji
Atmos. Chem. Phys., 19, 1059–1076, https://doi.org/10.5194/acp-19-1059-2019, https://doi.org/10.5194/acp-19-1059-2019, 2019
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The role non-mineral components play in the freezing behavior of atmospheric desert dust is not well known. In this study, we use chemical imaging methods to investigate this for airborne and surface-collected desert dust samples. We find that in most cases the ice nucleation behavior is determined by the dust mineralogical composition. However, volatile organic material can coat active sites and decrease the dust ice nucleation ability, while biological particles can significantly increase it.
Mikhail Paramonov, Robert O. David, Ruben Kretzschmar, and Zamin A. Kanji
Atmos. Chem. Phys., 18, 16515–16536, https://doi.org/10.5194/acp-18-16515-2018, https://doi.org/10.5194/acp-18-16515-2018, 2018
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The paper presents an overview of the ice nucleation activity of surface-collected mineral and soil dust. Emphasis is placed on disentangling the effects of mineral, biogenic and soluble components of the dust on its ice nucleation activity. The results revealed that it is not possible to predict the ice nucleation activity of the surface-collected dust based on the presence and amount of certain minerals or any particular class of compounds, such as soluble or proteinaceous/organic compounds.
Paul J. DeMott, Ottmar Möhler, Daniel J. Cziczo, Naruki Hiranuma, Markus D. Petters, Sarah S. Petters, Franco Belosi, Heinz G. Bingemer, Sarah D. Brooks, Carsten Budke, Monika Burkert-Kohn, Kristen N. Collier, Anja Danielczok, Oliver Eppers, Laura Felgitsch, Sarvesh Garimella, Hinrich Grothe, Paul Herenz, Thomas C. J. Hill, Kristina Höhler, Zamin A. Kanji, Alexei Kiselev, Thomas Koop, Thomas B. Kristensen, Konstantin Krüger, Gourihar Kulkarni, Ezra J. T. Levin, Benjamin J. Murray, Alessia Nicosia, Daniel O'Sullivan, Andreas Peckhaus, Michael J. Polen, Hannah C. Price, Naama Reicher, Daniel A. Rothenberg, Yinon Rudich, Gianni Santachiara, Thea Schiebel, Jann Schrod, Teresa M. Seifried, Frank Stratmann, Ryan C. Sullivan, Kaitlyn J. Suski, Miklós Szakáll, Hans P. Taylor, Romy Ullrich, Jesus Vergara-Temprado, Robert Wagner, Thomas F. Whale, Daniel Weber, André Welti, Theodore W. Wilson, Martin J. Wolf, and Jake Zenker
Atmos. Meas. Tech., 11, 6231–6257, https://doi.org/10.5194/amt-11-6231-2018, https://doi.org/10.5194/amt-11-6231-2018, 2018
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The ability to measure ice nucleating particles is vital to quantifying their role in affecting clouds and precipitation. Methods for measuring droplet freezing were compared while co-sampling relevant particle types. Measurement correspondence was very good for ice nucleating particles of bacterial and natural soil origin, and somewhat more disparate for those of mineral origin. Results reflect recently improved capabilities and provide direction toward addressing remaining measurement issues.
Emma Järvinen, Olivier Jourdan, David Neubauer, Bin Yao, Chao Liu, Meinrat O. Andreae, Ulrike Lohmann, Manfred Wendisch, Greg M. McFarquhar, Thomas Leisner, and Martin Schnaiter
Atmos. Chem. Phys., 18, 15767–15781, https://doi.org/10.5194/acp-18-15767-2018, https://doi.org/10.5194/acp-18-15767-2018, 2018
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Using light diffraction it is possible to detect microscopic features within ice particles that have not yet been fully characterized. Here, this technique was applied in airborne measurements, where it was found that majority of atmospheric ice particles have features that significantly change the way ice particles interact with solar light. The microscopic features make ice-containing clouds more reflective than previously thought, which could have consequences for predicting our climate.
Sarah Grawe, Stefanie Augustin-Bauditz, Hans-Christian Clemen, Martin Ebert, Stine Eriksen Hammer, Jasmin Lubitz, Naama Reicher, Yinon Rudich, Johannes Schneider, Robert Staacke, Frank Stratmann, André Welti, and Heike Wex
Atmos. Chem. Phys., 18, 13903–13923, https://doi.org/10.5194/acp-18-13903-2018, https://doi.org/10.5194/acp-18-13903-2018, 2018
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In this study, coal fly ash particles immersed in supercooled cloud droplets were analyzed concerning their freezing behavior. Additionally, physico-chemical particle properties (morphology, chemical composition, crystallography) were investigated. In combining both aspects, components that potentially contribute to the observed freezing behavior of the ash could be identified. Interactions at the particle-water interface, that depend on suspension time and influence freezing, are discussed.
Harri Kokkola, Thomas Kühn, Anton Laakso, Tommi Bergman, Kari E. J. Lehtinen, Tero Mielonen, Antti Arola, Scarlet Stadtler, Hannele Korhonen, Sylvaine Ferrachat, Ulrike Lohmann, David Neubauer, Ina Tegen, Colombe Siegenthaler-Le Drian, Martin G. Schultz, Isabelle Bey, Philip Stier, Nikos Daskalakis, Colette L. Heald, and Sami Romakkaniemi
Geosci. Model Dev., 11, 3833–3863, https://doi.org/10.5194/gmd-11-3833-2018, https://doi.org/10.5194/gmd-11-3833-2018, 2018
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In this paper we present a global aerosol–chemistry–climate model with the focus on its representation for atmospheric aerosol particles. In the model, aerosols are simulated using the aerosol module SALSA2.0, which in this paper is compared to satellite, ground, and aircraft-based observations of the properties of atmospheric aerosol. Based on this study, the model simulated aerosol properties compare well with the observations.
Fabian Mahrt, Claudia Marcolli, Robert O. David, Philippe Grönquist, Eszter J. Barthazy Meier, Ulrike Lohmann, and Zamin A. Kanji
Atmos. Chem. Phys., 18, 13363–13392, https://doi.org/10.5194/acp-18-13363-2018, https://doi.org/10.5194/acp-18-13363-2018, 2018
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The ice nucleation ability of different soot particles in the cirrus and mixed-phase cloud temperature regime is presented. The impact of aerosol particle size, particle morphology, organic matter and hydrophilicity on ice nucleation is examined. We propose ice nucleation proceeds via a pore condensation freezing mechanism for soot particles with the necessary physicochemical properties that nucleated ice well below water saturation.
Anina Gilgen, Carole Adolf, Sandra O. Brugger, Luisa Ickes, Margit Schwikowski, Jacqueline F. N. van Leeuwen, Willy Tinner, and Ulrike Lohmann
Atmos. Chem. Phys., 18, 11813–11829, https://doi.org/10.5194/acp-18-11813-2018, https://doi.org/10.5194/acp-18-11813-2018, 2018
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Microscopic charcoal particles are fire-specific tracers, which are presently the primary source for reconstructing past fire activity. In this study, we implement microscopic charcoal particles into a global aerosol–climate model to better understand the transport of charcoal on a large scale. We find that the model captures a significant portion of the spatial variability but fails to reproduce the extreme variability observed in the charcoal data.
Juliane L. Fry, Steven S. Brown, Ann M. Middlebrook, Peter M. Edwards, Pedro Campuzano-Jost, Douglas A. Day, José L. Jimenez, Hannah M. Allen, Thomas B. Ryerson, Ilana Pollack, Martin Graus, Carsten Warneke, Joost A. de Gouw, Charles A. Brock, Jessica Gilman, Brian M. Lerner, William P. Dubé, Jin Liao, and André Welti
Atmos. Chem. Phys., 18, 11663–11682, https://doi.org/10.5194/acp-18-11663-2018, https://doi.org/10.5194/acp-18-11663-2018, 2018
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This paper uses measurements made during research aircraft flights through power plant smokestack emissions plumes as a natural laboratory in the field experiment. We investigated a specific source of airborne particulate matter from the combination of human-produced NOx pollutant emissions (the smokestack plumes) with isoprene emitted by naturally by trees in the southeastern United States. These field-based yields appear to be higher than those typically measured in chamber studies.
Wan Ting Katty Huang, Luisa Ickes, Ina Tegen, Matteo Rinaldi, Darius Ceburnis, and Ulrike Lohmann
Atmos. Chem. Phys., 18, 11423–11445, https://doi.org/10.5194/acp-18-11423-2018, https://doi.org/10.5194/acp-18-11423-2018, 2018
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In this study, we investigated the potential impact on clouds and climate by organic particles emitted from the ocean surface, using a global climate model. These particles have previously been found to promote ice crystal formation, which may alter the properties of clouds. Our study, however, found a weak global impact by these particles, which brings into question their relative importance and points to the need for further verification with other models and at more regional scales.
Robin G. Stevens, Katharina Loewe, Christopher Dearden, Antonios Dimitrelos, Anna Possner, Gesa K. Eirund, Tomi Raatikainen, Adrian A. Hill, Benjamin J. Shipway, Jonathan Wilkinson, Sami Romakkaniemi, Juha Tonttila, Ari Laaksonen, Hannele Korhonen, Paul Connolly, Ulrike Lohmann, Corinna Hoose, Annica M. L. Ekman, Ken S. Carslaw, and Paul R. Field
Atmos. Chem. Phys., 18, 11041–11071, https://doi.org/10.5194/acp-18-11041-2018, https://doi.org/10.5194/acp-18-11041-2018, 2018
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We perform a model intercomparison of summertime high Arctic clouds. Observed concentrations of aerosol particles necessary for cloud formation fell to extremely low values, coincident with a transition from cloudy to nearly cloud-free conditions. Previous analyses have suggested that at these low concentrations, the radiative properties of the clouds are determined primarily by these particle concentrations. The model results strongly support this hypothesis.
Anina Gilgen, Wan Ting Katty Huang, Luisa Ickes, David Neubauer, and Ulrike Lohmann
Atmos. Chem. Phys., 18, 10521–10555, https://doi.org/10.5194/acp-18-10521-2018, https://doi.org/10.5194/acp-18-10521-2018, 2018
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Aerosol emissions in Arctic summer and autumn are expected to increase in the future because of sea ice retreat. Using a global aerosol–climate model, we quantify the impact of increased aerosol emissions from the ocean and from Arctic shipping in the year 2050. The influence on radiation of both aerosols and clouds is analysed. Mainly driven by changes in surface albedo, the cooling effect of marine aerosols and clouds will increase. Future ship emissions might have a small net cooling effect.
Alexander Beck, Jan Henneberger, Jacob P. Fugal, Robert O. David, Larissa Lacher, and Ulrike Lohmann
Atmos. Chem. Phys., 18, 8909–8927, https://doi.org/10.5194/acp-18-8909-2018, https://doi.org/10.5194/acp-18-8909-2018, 2018
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This study assesses the impact of surface processes (e.g. blowing snow) on in situ cloud observations at Sonnblick Observatory. Vertical profiles of ice crystal number concentrations (ICNCs) above a snow-covered surface were observed up to a height of 10 m. The ICNC near the ground is at least a factor of 2 larger than at 10 m. Therefore, in situ measurements of ICNCs at mountain-top research stations close to the surface are strongly influenced by surface processes and overestimate the ICNC.
Ulrike Lohmann and David Neubauer
Atmos. Chem. Phys., 18, 8807–8828, https://doi.org/10.5194/acp-18-8807-2018, https://doi.org/10.5194/acp-18-8807-2018, 2018
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The climate is warming, at the current rate so much so that the 2 ºC target is likely to be exceeded. Uncertainty remains as to when the 2 ºC of warming will be reached. One factor contributing to this uncertainty is how clouds change in the warmer climate. While previously most emphasis was placed on how low clouds change in the warmer climate, here we investigate the importance of mixed-phase and ice clouds.
Martin G. Schultz, Scarlet Stadtler, Sabine Schröder, Domenico Taraborrelli, Bruno Franco, Jonathan Krefting, Alexandra Henrot, Sylvaine Ferrachat, Ulrike Lohmann, David Neubauer, Colombe Siegenthaler-Le Drian, Sebastian Wahl, Harri Kokkola, Thomas Kühn, Sebastian Rast, Hauke Schmidt, Philip Stier, Doug Kinnison, Geoffrey S. Tyndall, John J. Orlando, and Catherine Wespes
Geosci. Model Dev., 11, 1695–1723, https://doi.org/10.5194/gmd-11-1695-2018, https://doi.org/10.5194/gmd-11-1695-2018, 2018
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The chemistry–climate model ECHAM-HAMMOZ contains a detailed representation of tropospheric and stratospheric reactive chemistry and state-of-the-art parameterizations of aerosols. It thus allows for detailed investigations of chemical processes in the climate system. Evaluation of the model with various observational data yields good results, but the model has a tendency to produce too much OH in the tropics. This highlights the important interplay between atmospheric chemistry and dynamics.
André Welti, Konrad Müller, Zoë L. Fleming, and Frank Stratmann
Atmos. Chem. Phys., 18, 5307–5320, https://doi.org/10.5194/acp-18-5307-2018, https://doi.org/10.5194/acp-18-5307-2018, 2018
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We report on ambient concentrations of ice nuclei, measured on the Cabo Verde islands. Concentrations are found to exponentially increase by 7 orders of magnitude from −5 to −38 °C. At each temperature, the frequency distribution of observed concentrations can be described by a lognormal distribution, typical for random dilution of substances during transport. Random dilution is found to account for larger fluctuations in IN concentration than seasonal changes and changes in air mass origin.
Remo Dietlicher, David Neubauer, and Ulrike Lohmann
Geosci. Model Dev., 11, 1557–1576, https://doi.org/10.5194/gmd-11-1557-2018, https://doi.org/10.5194/gmd-11-1557-2018, 2018
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A new cloud scheme was implemented in the aerosol–climate model ECHAM6-HAM2. Unlike traditional schemes, it does not categorize ice particles by in-cloud and precipitation types but uses a single category with prognostic bulk particle properties. The new scheme is not only conceptually simpler but also closer to first principles as it does not rely on weakly constrained conversion rates between predefined categories and resolves falling ice by local sub-time-stepping.
Larissa Lacher, Ulrike Lohmann, Yvonne Boose, Assaf Zipori, Erik Herrmann, Nicolas Bukowiecki, Martin Steinbacher, and Zamin A. Kanji
Atmos. Chem. Phys., 17, 15199–15224, https://doi.org/10.5194/acp-17-15199-2017, https://doi.org/10.5194/acp-17-15199-2017, 2017
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We characterize the new Horizontal Ice Nucleation Chamber HINC to measure ambient ice nucleating particle concentrations at mixed‐phase cloud conditions. Results from winter measurements at the High Altitude Research Station Jungfraujoch compare well to previous measurements. We find increased ice nucleating particle concentrations during the influence of Saharan dust events and marine events, which highlights the importance of these species on ice nucleation in the free troposphere.
David Neubauer, Matthew W. Christensen, Caroline A. Poulsen, and Ulrike Lohmann
Atmos. Chem. Phys., 17, 13165–13185, https://doi.org/10.5194/acp-17-13165-2017, https://doi.org/10.5194/acp-17-13165-2017, 2017
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When aerosol particles take up water their number may seem to be increased optically. However if aerosol particles are removed by precipitation (formation) their numbers will decrease. We applied methods to account for such effects in model and satellite data to analyse the change in cloud properties by changes in aerosol particle number. The agreement of model and satellite data improves when these effects are accounted for.
Jin Liao, Charles A. Brock, Daniel M. Murphy, Donna T. Sueper, André Welti, and Ann M. Middlebrook
Atmos. Meas. Tech., 10, 3801–3820, https://doi.org/10.5194/amt-10-3801-2017, https://doi.org/10.5194/amt-10-3801-2017, 2017
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The Aerodyne aerosol mass spectrometer (AMS) has emerged as a widely used method for measuring the real-time, submicron, nonrefractory aerosol composition. A large uncertainty in accurate measurements with the AMS (the collection efficiency due to particle bounce) is evaluated in this paper using in situ measurements of particle light scattering. Current calculations of the collection efficiency reasonably predict this effect in acidic environments, resulting in more confidence for AMS results.
Monika Burkert-Kohn, Heike Wex, André Welti, Susan Hartmann, Sarah Grawe, Lisa Hellner, Paul Herenz, James D. Atkinson, Frank Stratmann, and Zamin A. Kanji
Atmos. Chem. Phys., 17, 11683–11705, https://doi.org/10.5194/acp-17-11683-2017, https://doi.org/10.5194/acp-17-11683-2017, 2017
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Several instruments can investigate properties of ice-nucleating particles (INPs), which are crucial to understanding ice cloud formation. We intercompare four online ice nucleation counters and reasonable agreement is found when the same ice nucleation mode is tested. A variable scaling factor was necessary to reconcile condensation freezing results with immersion freezing. Factors related to instrumental setup and aerosol generation are discussed to explain observed differences.
Sarvesh Garimella, Daniel A. Rothenberg, Martin J. Wolf, Robert O. David, Zamin A. Kanji, Chien Wang, Michael Rösch, and Daniel J. Cziczo
Atmos. Chem. Phys., 17, 10855–10864, https://doi.org/10.5194/acp-17-10855-2017, https://doi.org/10.5194/acp-17-10855-2017, 2017
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This study investigates systematic and variable low bias in the measurement of ice nucleating particle concentration using continuous flow diffusion chambers. We find that non-ideal instrument behavior exposes particles to different humidities and/or temperatures than predicted from theory. We use a machine learning approach to quantify and minimize the uncertainty associated with this measurement bias.
Hendrik Andersen, Jan Cermak, Julia Fuchs, Reto Knutti, and Ulrike Lohmann
Atmos. Chem. Phys., 17, 9535–9546, https://doi.org/10.5194/acp-17-9535-2017, https://doi.org/10.5194/acp-17-9535-2017, 2017
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Aerosol-cloud interactions continue to contribute large uncertainties to our climate system understanding. In this study, we use near-global satellite and reanalysis data sets to predict marine liquid-water clouds by means of artificial neural networks. We show that on the system scale, lower-tropospheric stability and boundary layer height are the main determinants of liquid-water clouds. Aerosols show the expected impact on clouds but are less relevant than some meteorological factors.
Franziska Glassmeier, Anna Possner, Bernhard Vogel, Heike Vogel, and Ulrike Lohmann
Atmos. Chem. Phys., 17, 8651–8680, https://doi.org/10.5194/acp-17-8651-2017, https://doi.org/10.5194/acp-17-8651-2017, 2017
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We compare two chemistry and aerosol schemes – one designed for air-quality, the other for climate applications. For distribution, composition and radiative properties, the choice of aerosol types and processes turns out to be more important than their implementation. For aerosol–cloud interactions, we find cloud processes, in particular ice formation, to be the main obstacle to our understanding.
Anahita Amiri-Farahani, Robert J. Allen, David Neubauer, and Ulrike Lohmann
Atmos. Chem. Phys., 17, 6305–6322, https://doi.org/10.5194/acp-17-6305-2017, https://doi.org/10.5194/acp-17-6305-2017, 2017
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We use observations from 2004 to 2012 to obtain estimates of the aerosol–cloud radiative effect, including its uncertainty, for dust aerosol influencing Atlantic marine stratocumulus clouds (MSc) off the coast of north Africa. Saharan dust modifies MSc in a way that acts to cool the planet. There is a strong seasonal variation, with the aerosol–cloud radiative effect switching from significantly negative during the boreal summer to weakly positive during boreal winter.
Hanna Joos, Erica Madonna, Kasja Witlox, Sylvaine Ferrachat, Heini Wernli, and Ulrike Lohmann
Atmos. Chem. Phys., 17, 6243–6255, https://doi.org/10.5194/acp-17-6243-2017, https://doi.org/10.5194/acp-17-6243-2017, 2017
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The influence of pollution on the precipitation formation in warm conveyor belts (WCBs), the most rising air streams in low-pressure systems is investigated. We investigate in detail the cloud properties and resulting precipitation along these rising airstreams which are simulated with a global climate model. Overall, no big impact of aerosols on precipitation can be seen, however, when comparing the most polluted/cleanest WCBs, a suppression of precipitation by aerosols is observed.
Blaž Gasparini, Steffen Münch, Laure Poncet, Monika Feldmann, and Ulrike Lohmann
Atmos. Chem. Phys., 17, 4871–4885, https://doi.org/10.5194/acp-17-4871-2017, https://doi.org/10.5194/acp-17-4871-2017, 2017
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Cirrus clouds have, unlike other cloud types, a warming impact on climate. Decreasing their frequency therefore leads to a cooling effect. Cirrus ice crystals grow larger when formed on solid aerosols, inducing a shorter cloud lifetime.
We compare simplified simulations of stripping cirrus out of the sky with simulations of seeding by aerosol injections. While we find the surface climate responses to be similar, the changes in clouds and cloud properties differ significantly.
Alexander Beck, Jan Henneberger, Sarah Schöpfer, Jacob Fugal, and Ulrike Lohmann
Atmos. Meas. Tech., 10, 459–476, https://doi.org/10.5194/amt-10-459-2017, https://doi.org/10.5194/amt-10-459-2017, 2017
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In situ observations of cloud properties in complex alpine terrain are commonly conducted at mountain-top research stations and limited to single-point measurements. The HoloGondel platform overcomes this limitation by using a cable car to obtain vertical profiles of the microphysical and meteorological cloud parameters. In this work example measurements of the vertical profiles observed in a liquid cloud and a mixed-phase cloud at the Eggishorn in the Swiss Alps are presented.
Luisa Ickes, André Welti, and Ulrike Lohmann
Atmos. Chem. Phys., 17, 1713–1739, https://doi.org/10.5194/acp-17-1713-2017, https://doi.org/10.5194/acp-17-1713-2017, 2017
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The goal of this study is to find a parameterization scheme for general circulation models to describe immersion freezing with the ability to shift and adjust the slope of the freezing curve compared to homogeneous freezing to match experimental data. We investigated how accurate different formulations of classical nucleation theory reproduce measured immersion freezing curves for different mineral dust types.
Yvonne Boose, André Welti, James Atkinson, Fabiola Ramelli, Anja Danielczok, Heinz G. Bingemer, Michael Plötze, Berko Sierau, Zamin A. Kanji, and Ulrike Lohmann
Atmos. Chem. Phys., 16, 15075–15095, https://doi.org/10.5194/acp-16-15075-2016, https://doi.org/10.5194/acp-16-15075-2016, 2016
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We compare the immersion freezing behavior of four airborne to 11 surface-collected dust samples to investigate the role of different minerals for atmospheric ice nucleation on desert dust. We find that present K-feldspars dominate at T > 253 K, while quartz does at colder temperatures, and surface-collected dust samples are not necessarily representative for airborne dust. For improved ice cloud prediction, modeling of quartz and feldspar emission and transport are key.
Yvonne Boose, Berko Sierau, M. Isabel García, Sergio Rodríguez, Andrés Alastuey, Claudia Linke, Martin Schnaiter, Piotr Kupiszewski, Zamin A. Kanji, and Ulrike Lohmann
Atmos. Chem. Phys., 16, 9067–9087, https://doi.org/10.5194/acp-16-9067-2016, https://doi.org/10.5194/acp-16-9067-2016, 2016
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Mineral dust is known to be among the most prevalent ice-nucleating particles (INPs) in the atmosphere, playing a crucial role for ice cloud formation. We present 2 months of ground-based in situ measurements of INP concentrations in the free troposphere close to the largest global dust source, the Sahara. We find that some atmospheric processes such as mixing with biological particles and ammonium increase the dust INP ability. This is important when predicting INPs based on emissions.
Baban Nagare, Claudia Marcolli, André Welti, Olaf Stetzer, and Ulrike Lohmann
Atmos. Chem. Phys., 16, 8899–8914, https://doi.org/10.5194/acp-16-8899-2016, https://doi.org/10.5194/acp-16-8899-2016, 2016
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The relative importance of contact freezing and immersion freezing at mixed-phase cloud temperatures is the subject of debate. We performed experiments using continuous-flow diffusion chambers to compare the freezing efficiency of ice-nucleating particles for both these nucleation modes. Silver iodide, kaolinite and Arizona Test Dust were used as ice-nucleating particles. We could not confirm the dominance of contact freezing over immersion freezing for our experimental conditions.
Claudia Marcolli, Baban Nagare, André Welti, and Ulrike Lohmann
Atmos. Chem. Phys., 16, 8915–8937, https://doi.org/10.5194/acp-16-8915-2016, https://doi.org/10.5194/acp-16-8915-2016, 2016
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Silver iodide is one of the best-investigated ice nuclei. It has relevance for the atmosphere since it is used for glaciogenic cloud seeding. Nevertheless, many open questions remain. This paper gives an overview of silver iodide as an ice nucleus and tries to identify the factors that influence the ice nucleation ability of silver iodide.
Sarvesh Garimella, Thomas Bjerring Kristensen, Karolina Ignatius, Andre Welti, Jens Voigtländer, Gourihar R. Kulkarni, Frank Sagan, Gregory Lee Kok, James Dorsey, Leonid Nichman, Daniel Alexander Rothenberg, Michael Rösch, Amélie Catharina Ruth Kirchgäßner, Russell Ladkin, Heike Wex, Theodore W. Wilson, Luis Antonio Ladino, Jon P. D. Abbatt, Olaf Stetzer, Ulrike Lohmann, Frank Stratmann, and Daniel James Cziczo
Atmos. Meas. Tech., 9, 2781–2795, https://doi.org/10.5194/amt-9-2781-2016, https://doi.org/10.5194/amt-9-2781-2016, 2016
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The SPectrometer for Ice Nuclei (SPIN) is a commercially available ice nuclei counter manufactured by Droplet Measurement Technologies in Boulder, CO. This study characterizes the SPIN chamber, reporting data from laboratory measurements and quantifying uncertainties. Overall, we report that the SPIN is able to reproduce previous CFDC ice nucleation measurements.
Charles A. Brock, Nicholas L. Wagner, Bruce E. Anderson, Alexis R. Attwood, Andreas Beyersdorf, Pedro Campuzano-Jost, Annmarie G. Carlton, Douglas A. Day, Glenn S. Diskin, Timothy D. Gordon, Jose L. Jimenez, Daniel A. Lack, Jin Liao, Milos Z. Markovic, Ann M. Middlebrook, Nga L. Ng, Anne E. Perring, Matthews S. Richardson, Joshua P. Schwarz, Rebecca A. Washenfelder, Andre Welti, Lu Xu, Luke D. Ziemba, and Daniel M. Murphy
Atmos. Chem. Phys., 16, 4987–5007, https://doi.org/10.5194/acp-16-4987-2016, https://doi.org/10.5194/acp-16-4987-2016, 2016
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Microscopic pollution particles make the atmosphere look hazy and also cool the earth by sending sunlight back to space. When the air is moist, these particles swell with water and scatter even more sunlight. We showed that particles formed from organic material – which dominates particulate pollution in the southeastern U.S. – does not take up water very effectively, toward the low end of most previous studies. We also found a better way to mathematically describe this swelling process.
Charles A. Brock, Nicholas L. Wagner, Bruce E. Anderson, Andreas Beyersdorf, Pedro Campuzano-Jost, Douglas A. Day, Glenn S. Diskin, Timothy D. Gordon, Jose L. Jimenez, Daniel A. Lack, Jin Liao, Milos Z. Markovic, Ann M. Middlebrook, Anne E. Perring, Matthews S. Richardson, Joshua P. Schwarz, Andre Welti, Luke D. Ziemba, and Daniel M. Murphy
Atmos. Chem. Phys., 16, 5009–5019, https://doi.org/10.5194/acp-16-5009-2016, https://doi.org/10.5194/acp-16-5009-2016, 2016
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Two research aircraft made dozens of vertical profiles over rural areas in the southeastern US in summer 2013. These measurements show that, in addition to how much pollution was present and how moist the atmosphere was, the size of the pollutant particles affected how much sunlight was reflected back to space. These measurements will help climate modelers determine which characteristics of pollution are important to predict with accuracy.
Shipeng Zhang, Minghuai Wang, Steven J. Ghan, Aijun Ding, Hailong Wang, Kai Zhang, David Neubauer, Ulrike Lohmann, Sylvaine Ferrachat, Toshihiko Takeamura, Andrew Gettelman, Hugh Morrison, Yunha Lee, Drew T. Shindell, Daniel G. Partridge, Philip Stier, Zak Kipling, and Congbin Fu
Atmos. Chem. Phys., 16, 2765–2783, https://doi.org/10.5194/acp-16-2765-2016, https://doi.org/10.5194/acp-16-2765-2016, 2016
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The variation of aerosol indirect effects (AIE) in several climate models is investigated across different dynamical regimes. Regimes with strong large-scale ascent are shown to be as important as stratocumulus regimes in studying AIE. AIE over regions with high monthly large-scale surface precipitation rate contributes the most to the total aerosol indirect forcing. These results point to the need to reduce the uncertainty in AIE in different dynamical regimes.
R. H. Mason, M. Si, C. Chou, V. E. Irish, R. Dickie, P. Elizondo, R. Wong, M. Brintnell, M. Elsasser, W. M. Lassar, K. M. Pierce, W. R. Leaitch, A. M. MacDonald, A. Platt, D. Toom-Sauntry, R. Sarda-Estève, C. L. Schiller, K. J. Suski, T. C. J. Hill, J. P. D. Abbatt, J. A. Huffman, P. J. DeMott, and A. K. Bertram
Atmos. Chem. Phys., 16, 1637–1651, https://doi.org/10.5194/acp-16-1637-2016, https://doi.org/10.5194/acp-16-1637-2016, 2016
B. Nagare, C. Marcolli, O. Stetzer, and U. Lohmann
Atmos. Chem. Phys., 15, 13759–13776, https://doi.org/10.5194/acp-15-13759-2015, https://doi.org/10.5194/acp-15-13759-2015, 2015
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We determined collision efficiencies of cloud droplets with aerosol particles experimentally and found that they were around 1 order of magnitude higher than theoretical formulations that include Brownian diffusion, impaction, interception, thermophoretic, diffusiophoretic and electric forces. This is most probably due to uncertainties and inaccuracies in the theoretical formulations of thermophoretic and diffusiophoretic processes.
R. H. Mason, M. Si, J. Li, C. Chou, R. Dickie, D. Toom-Sauntry, C. Pöhlker, J. D. Yakobi-Hancock, L. A. Ladino, K. Jones, W. R. Leaitch, C. L. Schiller, J. P. D. Abbatt, J. A. Huffman, and A. K. Bertram
Atmos. Chem. Phys., 15, 12547–12566, https://doi.org/10.5194/acp-15-12547-2015, https://doi.org/10.5194/acp-15-12547-2015, 2015
M. Paramonov, V.-M. Kerminen, M. Gysel, P. P. Aalto, M. O. Andreae, E. Asmi, U. Baltensperger, A. Bougiatioti, D. Brus, G. P. Frank, N. Good, S. S. Gunthe, L. Hao, M. Irwin, A. Jaatinen, Z. Jurányi, S. M. King, A. Kortelainen, A. Kristensson, H. Lihavainen, M. Kulmala, U. Lohmann, S. T. Martin, G. McFiggans, N. Mihalopoulos, A. Nenes, C. D. O'Dowd, J. Ovadnevaite, T. Petäjä, U. Pöschl, G. C. Roberts, D. Rose, B. Svenningsson, E. Swietlicki, E. Weingartner, J. Whitehead, A. Wiedensohler, C. Wittbom, and B. Sierau
Atmos. Chem. Phys., 15, 12211–12229, https://doi.org/10.5194/acp-15-12211-2015, https://doi.org/10.5194/acp-15-12211-2015, 2015
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The research paper presents the first comprehensive overview of field measurements with the CCN Counter performed at a large number of locations around the world within the EUCAARI framework. The paper sheds light on the CCN number concentrations and activated fractions around the world and their dependence on the water vapour supersaturation ratio, the dependence of aerosol hygroscopicity on particle size, and seasonal and diurnal variation of CCN activation and hygroscopic properties.
J. C. Corbin, A. Othman, J. D. Allan, D. R. Worsnop, J. D. Haskins, B. Sierau, U. Lohmann, and A. A. Mensah
Atmos. Meas. Tech., 8, 4615–4636, https://doi.org/10.5194/amt-8-4615-2015, https://doi.org/10.5194/amt-8-4615-2015, 2015
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Peak-integration uncertainties in the Aerodyne high-resolution aerosol mass spectrometer (AMS) are analyzed in detail using a combination of empirical data analysis and Monte Carlo approaches. The most general conclusion, applicable to any mass spectrometer, is that non-zero mass accuracy leads to a percentage error in constrained peak fits, even for well-resolved peaks. For overlapping peaks, this mass-accuracy effect may be viewed as a reduction in the effective m/z-calibration precision.
J. C. Corbin, U. Lohmann, B. Sierau, A. Keller, H. Burtscher, and A. A. Mensah
Atmos. Chem. Phys., 15, 11885–11907, https://doi.org/10.5194/acp-15-11885-2015, https://doi.org/10.5194/acp-15-11885-2015, 2015
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The chemical composition of wood-combustion soot is investigated using a soot-particle aerosol mass spectrometer. The analysis elucidates real-time information on BC oxygenated surface functional groups for a real-world source for the first time. Additional insights into the source of organic material in this soot are provided by positive matrix factorization of the data using a new AMS error model.
P. S. Kim, D. J. Jacob, J. A. Fisher, K. Travis, K. Yu, L. Zhu, R. M. Yantosca, M. P. Sulprizio, J. L. Jimenez, P. Campuzano-Jost, K. D. Froyd, J. Liao, J. W. Hair, M. A. Fenn, C. F. Butler, N. L. Wagner, T. D. Gordon, A. Welti, P. O. Wennberg, J. D. Crounse, J. M. St. Clair, A. P. Teng, D. B. Millet, J. P. Schwarz, M. Z. Markovic, and A. E. Perring
Atmos. Chem. Phys., 15, 10411–10433, https://doi.org/10.5194/acp-15-10411-2015, https://doi.org/10.5194/acp-15-10411-2015, 2015
E. Hammer, N. Bukowiecki, B. P. Luo, U. Lohmann, C. Marcolli, E. Weingartner, U. Baltensperger, and C. R. Hoyle
Atmos. Chem. Phys., 15, 10309–10323, https://doi.org/10.5194/acp-15-10309-2015, https://doi.org/10.5194/acp-15-10309-2015, 2015
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An important quantity which determines aerosol activation and cloud formation is the effective peak supersaturation. The box model ZOMM was used to simulate the effective peak supersaturation experienced by an air parcel approaching a high-alpine research station in Switzerland. With the box model the sensitivity of the effective peak supersaturation to key aerosol and dynamical parameters was investigated.
S. Pousse-Nottelmann, E. M. Zubler, and U. Lohmann
Atmos. Chem. Phys., 15, 9217–9236, https://doi.org/10.5194/acp-15-9217-2015, https://doi.org/10.5194/acp-15-9217-2015, 2015
V. Sant, R. Posselt, and U. Lohmann
Atmos. Chem. Phys., 15, 8717–8738, https://doi.org/10.5194/acp-15-8717-2015, https://doi.org/10.5194/acp-15-8717-2015, 2015
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We have introduced prognostic precipitation for both liquid (drizzle and rain) and solid (snow) phase precipitation into the global circulation model ECHAM5-HAM. This has a significant effect on the clouds and the parameterized collection rates, also reducing the sensitivity of the liquid water path to the anthropogenic aerosol forcing. Altogether the results suggest that the treatment of precipitation in global circulation models has a significant influence on the phase and lifetime of clouds.
S. Fuzzi, U. Baltensperger, K. Carslaw, S. Decesari, H. Denier van der Gon, M. C. Facchini, D. Fowler, I. Koren, B. Langford, U. Lohmann, E. Nemitz, S. Pandis, I. Riipinen, Y. Rudich, M. Schaap, J. G. Slowik, D. V. Spracklen, E. Vignati, M. Wild, M. Williams, and S. Gilardoni
Atmos. Chem. Phys., 15, 8217–8299, https://doi.org/10.5194/acp-15-8217-2015, https://doi.org/10.5194/acp-15-8217-2015, 2015
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Particulate matter (PM) constitutes one of the most challenging problems both for air quality and climate change policies. This paper reviews the most recent scientific results on the issue and the policy needs that have driven much of the increase in monitoring and mechanistic research over the last 2 decades. The synthesis reveals many new processes and developments in the science underpinning climate-PM interactions and the effects of PM on human health and the environment.
N. L. Wagner, C. A. Brock, W. M. Angevine, A. Beyersdorf, P. Campuzano-Jost, D. Day, J. A. de Gouw, G. S. Diskin, T. D. Gordon, M. G. Graus, J. S. Holloway, G. Huey, J. L. Jimenez, D. A. Lack, J. Liao, X. Liu, M. Z. Markovic, A. M. Middlebrook, T. Mikoviny, J. Peischl, A. E. Perring, M. S. Richardson, T. B. Ryerson, J. P. Schwarz, C. Warneke, A. Welti, A. Wisthaler, L. D. Ziemba, and D. M. Murphy
Atmos. Chem. Phys., 15, 7085–7102, https://doi.org/10.5194/acp-15-7085-2015, https://doi.org/10.5194/acp-15-7085-2015, 2015
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This paper investigates the summertime vertical profile of aerosol over the southeastern US using in situ measurements collected from aircraft. We use a vertical mixing model and measurements of CO to predict the vertical profile of aerosol that we would expect from vertical mixing alone and compare with the observed aerosol profile. We found a modest enhancement of aerosol in the cloudy transition layer during shallow cumulus convection and attribute the enhancement to local aerosol formation.
R. H. Mason, C. Chou, C. S. McCluskey, E. J. T. Levin, C. L. Schiller, T. C. J. Hill, J. A. Huffman, P. J. DeMott, and A. K. Bertram
Atmos. Meas. Tech., 8, 2449–2462, https://doi.org/10.5194/amt-8-2449-2015, https://doi.org/10.5194/amt-8-2449-2015, 2015
N. Hiranuma, S. Augustin-Bauditz, H. Bingemer, C. Budke, J. Curtius, A. Danielczok, K. Diehl, K. Dreischmeier, M. Ebert, F. Frank, N. Hoffmann, K. Kandler, A. Kiselev, T. Koop, T. Leisner, O. Möhler, B. Nillius, A. Peckhaus, D. Rose, S. Weinbruch, H. Wex, Y. Boose, P. J. DeMott, J. D. Hader, T. C. J. Hill, Z. A. Kanji, G. Kulkarni, E. J. T. Levin, C. S. McCluskey, M. Murakami, B. J. Murray, D. Niedermeier, M. D. Petters, D. O'Sullivan, A. Saito, G. P. Schill, T. Tajiri, M. A. Tolbert, A. Welti, T. F. Whale, T. P. Wright, and K. Yamashita
Atmos. Chem. Phys., 15, 2489–2518, https://doi.org/10.5194/acp-15-2489-2015, https://doi.org/10.5194/acp-15-2489-2015, 2015
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Seventeen ice nucleation measurement techniques contributed to investigate the immersion freezing behavior of illite NX. All data showed a similar temperature trend, but the measured ice nucleation activity was on average smaller for the wet suspended samples and higher for the dry-dispersed aerosol samples at high temperatures. A continued investigation and collaboration is necessary to obtain further insights into consistency or diversity of ice nucleation measurements.
A. Possner, E. Zubler, U. Lohmann, and C. Schär
Atmos. Chem. Phys., 15, 2185–2201, https://doi.org/10.5194/acp-15-2185-2015, https://doi.org/10.5194/acp-15-2185-2015, 2015
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For the first time, real-case simulations of ship tracks are performed at the 2km scale and evaluated against observations. Simulations show that ship tracks are quantitatively and qualitatively captured by the model. Therefore, this approach could be used to evaluate the interplay between parameterisations for aerosol–cloud interactions which occur, in the case of ship tracks, in spatially defined regions and under constrained environmental conditions.
H. Wex, S. Augustin-Bauditz, Y. Boose, C. Budke, J. Curtius, K. Diehl, A. Dreyer, F. Frank, S. Hartmann, N. Hiranuma, E. Jantsch, Z. A. Kanji, A. Kiselev, T. Koop, O. Möhler, D. Niedermeier, B. Nillius, M. Rösch, D. Rose, C. Schmidt, I. Steinke, and F. Stratmann
Atmos. Chem. Phys., 15, 1463–1485, https://doi.org/10.5194/acp-15-1463-2015, https://doi.org/10.5194/acp-15-1463-2015, 2015
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Immersion freezing measurements from seven different measurement techniques were intercompared using a biological ice nucleating material from bacteria. Although different techniques examined differently concentrated droplets, it was possible to find a uniform description, which showed that results from all experiments were generally in good agreement and were also in agreement with parameterizations published earlier in literature.
D. Neubauer, U. Lohmann, C. Hoose, and M. G. Frontoso
Atmos. Chem. Phys., 14, 11997–12022, https://doi.org/10.5194/acp-14-11997-2014, https://doi.org/10.5194/acp-14-11997-2014, 2014
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Several biases in the representation of clouds in the stratocumulus regime in the ECHAM6-HAM2 global climate model were found by evaluating the model in the stratocumulus cloud regime. Simulations with changes in model resolution and physics to better represent clouds and aerosol in the stratocumulus regime show that the human influence on clouds and thus climate by emission of aerosol particles is sensitive to the representation of (stratocumulus) clouds.
B. Sierau, R. Y.-W. Chang, C. Leck, J. Paatero, and U. Lohmann
Atmos. Chem. Phys., 14, 7409–7430, https://doi.org/10.5194/acp-14-7409-2014, https://doi.org/10.5194/acp-14-7409-2014, 2014
M. Kuebbeler, U. Lohmann, J. Hendricks, and B. Kärcher
Atmos. Chem. Phys., 14, 3027–3046, https://doi.org/10.5194/acp-14-3027-2014, https://doi.org/10.5194/acp-14-3027-2014, 2014
M. Tjernström, C. Leck, C. E. Birch, J. W. Bottenheim, B. J. Brooks, I. M. Brooks, L. Bäcklin, R. Y.-W. Chang, G. de Leeuw, L. Di Liberto, S. de la Rosa, E. Granath, M. Graus, A. Hansel, J. Heintzenberg, A. Held, A. Hind, P. Johnston, J. Knulst, M. Martin, P. A. Matrai, T. Mauritsen, M. Müller, S. J. Norris, M. V. Orellana, D. A. Orsini, J. Paatero, P. O. G. Persson, Q. Gao, C. Rauschenberg, Z. Ristovski, J. Sedlar, M. D. Shupe, B. Sierau, A. Sirevaag, S. Sjogren, O. Stetzer, E. Swietlicki, M. Szczodrak, P. Vaattovaara, N. Wahlberg, M. Westberg, and C. R. Wheeler
Atmos. Chem. Phys., 14, 2823–2869, https://doi.org/10.5194/acp-14-2823-2014, https://doi.org/10.5194/acp-14-2823-2014, 2014
J. C. Corbin, B. Sierau, M. Gysel, M. Laborde, A. Keller, J. Kim, A. Petzold, T. B. Onasch, U. Lohmann, and A. A. Mensah
Atmos. Chem. Phys., 14, 2591–2603, https://doi.org/10.5194/acp-14-2591-2014, https://doi.org/10.5194/acp-14-2591-2014, 2014
A. Baklanov, K. Schlünzen, P. Suppan, J. Baldasano, D. Brunner, S. Aksoyoglu, G. Carmichael, J. Douros, J. Flemming, R. Forkel, S. Galmarini, M. Gauss, G. Grell, M. Hirtl, S. Joffre, O. Jorba, E. Kaas, M. Kaasik, G. Kallos, X. Kong, U. Korsholm, A. Kurganskiy, J. Kushta, U. Lohmann, A. Mahura, A. Manders-Groot, A. Maurizi, N. Moussiopoulos, S. T. Rao, N. Savage, C. Seigneur, R. S. Sokhi, E. Solazzo, S. Solomos, B. Sørensen, G. Tsegas, E. Vignati, B. Vogel, and Y. Zhang
Atmos. Chem. Phys., 14, 317–398, https://doi.org/10.5194/acp-14-317-2014, https://doi.org/10.5194/acp-14-317-2014, 2014
J. Henneberger, J. P. Fugal, O. Stetzer, and U. Lohmann
Atmos. Meas. Tech., 6, 2975–2987, https://doi.org/10.5194/amt-6-2975-2013, https://doi.org/10.5194/amt-6-2975-2013, 2013
L. A. Ladino Moreno, O. Stetzer, and U. Lohmann
Atmos. Chem. Phys., 13, 9745–9769, https://doi.org/10.5194/acp-13-9745-2013, https://doi.org/10.5194/acp-13-9745-2013, 2013
C. Chou, Z. A. Kanji, O. Stetzer, T. Tritscher, R. Chirico, M. F. Heringa, E. Weingartner, A. S. H. Prévôt, U. Baltensperger, and U. Lohmann
Atmos. Chem. Phys., 13, 761–772, https://doi.org/10.5194/acp-13-761-2013, https://doi.org/10.5194/acp-13-761-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Boosting aerosol surface effects: strongly enhanced cooperative surface propensity of atmospherically relevant organic molecular ions in aqueous solution
The lifetimes and potential change in planetary albedo owing to the oxidation of thin surfactant organic films extracted from atmospheric aerosol by hydroxyl (OH) radicals at the air–water interface of particles
Exometabolomic exploration of culturable airborne microorganisms from an urban atmosphere
Measurement Report: Changes in ammonia emissions since the 18th century in south-eastern Europe inferred from an Elbrus (Caucasus, Russia) ice-core record
Atmospheric oxidation of 1,3-butadiene: influence of seed aerosol acidity and relative humidity on SOA composition and the production of air toxic compounds
Enhanced sulfate formation in mixed biomass burning and sea-salt interactions mediated by photosensitization: effects of chloride, nitrogen-containing compounds, and atmospheric aging
Heterogeneous formation and light absorption of secondary organic aerosols from acetone photochemical reactions: remarkably enhancing effects of seeds and ammonia
Experimental observation of the impact of nanostructure on hygroscopicity and reactivity of fatty acid atmospheric aerosol proxies
Technical note: High-resolution analyses of concentrations and sizes of refractory black carbon particles deposited in northwestern Greenland over the past 350 years – Part 1: Continuous flow analysis of the SIGMA-D ice core using the wide-range Single-Particle Soot Photometer and a high-efficiency nebulizer
The role of surface-active macromolecules in the ice nucleating ability of lignin, Snomax, and agricultural soil extracts
Particulate emissions from cooking: emission factors, emission dynamics, and mass spectrometric analysis for different cooking methods
Hydrogen Peroxide Photoformation in Particulate Matter and its Contribution to S(IV) Oxidation During Winter in Fairbanks, Alaska
Heterogeneous Phototransformation of Halogenated Polycyclic Aromatic Hydrocarbons: Influencing Factors, Mechanisms and Products
Nocturnal atmospheric synergistic oxidation reduces the formation of low-volatility organic compounds from biogenic emissions
The interplay between aqueous replacement reaction and the phase state of internally mixed organic/ammonium aerosols
Measurement report: The Fifth International Workshop on Ice Nucleation phase 1 (FIN-01): intercomparison of single-particle mass spectrometers
The importance of burning conditions on the composition of domestic biomass burning organic aerosol and the impact of atmospheric aging
Characterization of the particle size distribution, mineralogy, and Fe mode of occurrence of dust-emitting sediments from the Mojave Desert, California, USA
Measurement report: Effects of transition metal ions on the optical properties of humic-like substances (HULIS) reveal a structural preference – a case study of PM2.5 in Beijing, China
Probing Iceland's dust-emitting sediments: particle size distribution, mineralogy, cohesion, Fe mode of occurrence, and reflectance spectra signatures
Photoenhanced sulfate formation by the heterogeneous uptake of SO2 on non-photoactive mineral dust
Comparison of water-soluble and water-insoluble organic compositions attributing to different light absorption efficiency between residential coal and biomass burning emissions
Suppressed atmospheric chemical aging of cooking organic aerosol particles in wintertime conditions
Formation and loss of light absorbance by phenolic aqueous SOA by ●OH and an organic triplet excited state
Technical Note: A technique to convert NO2 to NO2− with S(IV) and its application to measuring nitrate photolysis
Distribution, chemical, and molecular composition of high and low molecular weight humic-like substances in ambient aerosols
Desorption lifetimes and activation energies influencing gas–surface interactions and multiphase chemical kinetics
Molecular analysis of secondary organic aerosol and brown carbon from the oxidation of indole
Secondary organic aerosol formed by Euro 5 gasoline vehicle emissions: chemical composition and gas-to-particle phase partitioning
Assessment of the contribution of residential waste burning to ambient PM10 concentrations in Hungary and Romania
Source differences in the components and cytotoxicity of PM2.5 from automobile exhaust, coal combustion, and biomass burning contributing to urban aerosol toxicity
Chamber studies of OH + dimethyl sulfoxide and dimethyl disulfide: insights into the dimethyl sulfide oxidation mechanism
Low-temperature ice nucleation of sea spray and secondary marine aerosols under cirrus cloud conditions
Temperature-dependent aqueous OH kinetics of C2–C10 linear and terpenoid alcohols and diols: new rate coefficients, structure–activity relationship, and atmospheric lifetimes
A possible unaccounted source of nitrogen-containing compound formation in aerosols: amines reacting with secondary ozonides
Seasonal variations in photooxidant formation and light absorption in aqueous extracts of ambient particles
Variability in sediment particle size, mineralogy, and Fe mode of occurrence across dust-source inland drainage basins: the case of the lower Drâa Valley, Morocco
Gas–particle partitioning of toluene oxidation products: an experimental and modeling study
Chemically speciated air pollutant emissions from open burning of household solid waste from South Africa
Bulk and molecular-level composition of primary organic aerosol from wood, straw, cow dung, and plastic burning
Volatile oxidation products and secondary organosiloxane aerosol from D5 + OH at varying OH exposures
Molecular fingerprints and health risks of smoke from home-use incense burning
High enrichment of heavy metals in fine particulate matter through dust aerosol generation
Production of ice-nucleating particles (INPs) by fast-growing phytoplankton
Technical note: In situ measurements and modelling of the oxidation kinetics in films of a cooking aerosol proxy using a quartz crystal microbalance with dissipation monitoring (QCM-D)
Contrasting impacts of humidity on the ozonolysis of monoterpenes: insights into the multi-generation chemical mechanism
Quantifying the seasonal variations in and regional transport of PM2.5 in the Yangtze River Delta region, China: characteristics, sources, and health risks
Opinion: Atmospheric multiphase chemistry – past, present, and future
Distinct photochemistry in glycine particles mixed with different atmospheric nitrate salts
Effects of storage conditions on the molecular-level composition of organic aerosol particles
Harmanjot Kaur, Stephan Thürmer, Shirin Gholami, Bruno Credidio, Florian Trinter, Debora Vasconcelos, Ricardo Marinho, Joel Pinheiro, Hendrik Bluhm, Arnaldo Naves de Brito, Gunnar Öhrwall, Bernd Winter, and Olle Björneholm
Atmos. Chem. Phys., 25, 3503–3518, https://doi.org/10.5194/acp-25-3503-2025, https://doi.org/10.5194/acp-25-3503-2025, 2025
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Understanding the surface composition of aerosols is crucial for advancing climate models. We investigated the interface of single-component and mixed aqueous solutions of atmospherically relevant carboxylic acid and alkyl-ammonium ions using liquid-jet photoelectron spectroscopy. An exponential increase in surface propensity as a function of chain length was found for the single species, and cooperative effects in the mixtures cause a further drastic increase in surface solute concentration.
Rosalie H. Shepherd, Martin D. King, Andrew D. Ward, Edward J. Stuckey, Rebecca J. L. Welbourn, Neil Brough, Adam Milsom, Christian Pfrang, and Thomas Arnold
Atmos. Chem. Phys., 25, 2569–2588, https://doi.org/10.5194/acp-25-2569-2025, https://doi.org/10.5194/acp-25-2569-2025, 2025
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Thin film formation at the air–water interface from material extracted from atmospheric aerosol was demonstrated, supporting the core–shell morphology. Film thicknesses were approximately 10 Å and 17 Å for urban and remote extracts, respectively. Exposure to gas-phase OH radicals showed fast reactions and short lifetimes of around 1 h. The effect on the Earth's radiative balance indicated that removing half of the film could significantly increase the top-of-atmosphere albedo for urban films.
Rui Jin, Wei Hu, Peimin Duan, Ming Sheng, Dandan Liu, Ziye Huang, Mutong Niu, Libin Wu, Junjun Deng, and Pingqing Fu
Atmos. Chem. Phys., 25, 1805–1829, https://doi.org/10.5194/acp-25-1805-2025, https://doi.org/10.5194/acp-25-1805-2025, 2025
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The metabolic capacity of atmospheric microorganisms after settling into habitats is poorly understood. We studied the molecular composition of exometabolites for cultured typical airborne microbes and traced their metabolic processes. Bacteria and fungi produce highly oxidized exometabolites and have significant variations in metabolism among different strains. These insights are pivotal for assessing the biogeochemical impacts of atmospheric microorganisms following their deposition.
Michel Legrand, Mstislav Vorobyev, Daria Bokuchava, Stanislav Kutuzov, Andreas Plach, Andreas Stohl, Alexandra Khairedinova, Vladimir Mikhalenko, Maria Vinogradova, Sabine Eckhardt, and Susanne Preunkert
Atmos. Chem. Phys., 25, 1385–1399, https://doi.org/10.5194/acp-25-1385-2025, https://doi.org/10.5194/acp-25-1385-2025, 2025
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Past atmospheric NH3 pollution in south-eastern Europe was reconstructed by analysing ammonium in an ice core drilled at the Mount Elbrus (Caucasus, Russia). The observed 3.5-fold increase in ice concentrations between 1750 and 1990 CE is in good agreement with estimated past dominant ammonia emissions from agriculture, mainly from south European Russia and Türkiye. In contrast to present-day conditions, the ammonium level observed in 1750 CE indicates significant natural emissions at that time.
Mohammed Jaoui, Klara Nestorowicz, Krzysztof J. Rudzinski, Michael Lewandowski, Tadeusz E. Kleindienst, Julio Torres, Ewa Bulska, Witold Danikiewicz, and Rafal Szmigielski
Atmos. Chem. Phys., 25, 1401–1432, https://doi.org/10.5194/acp-25-1401-2025, https://doi.org/10.5194/acp-25-1401-2025, 2025
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Recent research has established the contribution of 1,3-butadiene (13BD) to organic aerosol formation with negative implications for urban air quality. Health effect studies have focused on whole particulate matter, but compounds responsible for adverse health effects remain uncertain. This study provides the effect of relative humidity and seed aerosol acidity on the chemical composition of aerosol formed from 13BD photooxidation.
Rongzhi Tang, Jialiang Ma, Ruifeng Zhang, Weizhen Cui, Yuanyuan Qin, Yangxi Chu, Yiming Qin, Alexander L. Vogel, and Chak K. Chan
Atmos. Chem. Phys., 25, 425–439, https://doi.org/10.5194/acp-25-425-2025, https://doi.org/10.5194/acp-25-425-2025, 2025
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This study provides laboratory evidence that the photosensitizers in biomass burning extracts can enhance sulfate formation in NaCl particles, primarily by triggering the formation of secondary oxidants under light and air conditions, with a lower contribution of direct photosensitization via triplets.
Si Zhang, Yining Gao, Xinbei Xu, Luyao Chen, Can Wu, Zheng Li, Rongjie Li, Binyu Xiao, Xiaodi Liu, Rui Li, Fan Zhang, and Gehui Wang
Atmos. Chem. Phys., 24, 14177–14190, https://doi.org/10.5194/acp-24-14177-2024, https://doi.org/10.5194/acp-24-14177-2024, 2024
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Secondary organic aerosols (SOAs) from acetone photooxidation in the presence of various seeds were studied to illustrate SOA formation kinetics under ammonia-rich conditions. The oxidation mechanism of acetone was investigated using an observation-based model incorporating a Master Chemical Mechanism model. A higher SOA yield of acetone was observed compared to methylglyoxal due to an enhanced uptake of the small photooxidation products of acetone.
Adam Milsom, Adam M. Squires, Ben Laurence, Ben Wōden, Andrew J. Smith, Andrew D. Ward, and Christian Pfrang
Atmos. Chem. Phys., 24, 13571–13586, https://doi.org/10.5194/acp-24-13571-2024, https://doi.org/10.5194/acp-24-13571-2024, 2024
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We followed nano-structural changes in mixtures found in urban organic aerosol emissions (oleic acid, sodium oleate and fructose) during humidity change and ozone exposure. We demonstrate that self-assembly of fatty acid nanostructures can impact water uptake and chemical reactivity, affecting atmospheric lifetimes, urban air quality (preventing harmful emissions from degradation and enabling their long-range transport) and climate (affecting cloud formation), with implications for human health.
Kumiko Goto-Azuma, Remi Dallmayr, Yoshimi Ogawa-Tsukagawa, Nobuhiro Moteki, Tatsuhiro Mori, Sho Ohata, Yutaka Kondo, Makoto Koike, Motohiro Hirabayashi, Jun Ogata, Kyotaro Kitamura, Kenji Kawamura, Koji Fujita, Sumito Matoba, Naoko Nagatsuka, Akane Tsushima, Kaori Fukuda, and Teruo Aoki
Atmos. Chem. Phys., 24, 12985–13000, https://doi.org/10.5194/acp-24-12985-2024, https://doi.org/10.5194/acp-24-12985-2024, 2024
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We developed a continuous flow analysis system to analyze an ice core from northwestern Greenland and coupled it with an improved refractory black carbon (rBC) measurement technique. This allowed accurate high-resolution analyses of size distributions and concentrations of rBC particles with diameters of 70 nm–4 μm for the past 350 years. Our results provide crucial insights into rBC's climatic effects. We also found previous ice core studies substantially underestimated rBC mass concentrations.
Kathleen A. Thompson, Paul Bieber, Anna J. Miller, Nicole Link, Benjamin J. Murray, and Nadine Borduas-Dedekind
EGUsphere, https://doi.org/10.5194/egusphere-2024-2827, https://doi.org/10.5194/egusphere-2024-2827, 2024
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Lignin and Snomax are surface-active macromolecules that show a relationship between increasing concentrations, decreasing surface tension, and increasing ice-nucleating ability. However, this relationship did not hold for agricultural soil extracts collected in the UK and Canada. Hydrophobic interfaces play an important role in the ice-nucleating activity of organic matter; as the complexity of the sample increases, the hydrophobic interfaces in the bulk compete with the air-water interface.
Julia Pikmann, Frank Drewnick, Friederike Fachinger, and Stephan Borrmann
Atmos. Chem. Phys., 24, 12295–12321, https://doi.org/10.5194/acp-24-12295-2024, https://doi.org/10.5194/acp-24-12295-2024, 2024
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Cooking activities can contribute substantially to indoor and ambient aerosol. We performed a comprehensive study with laboratory measurements cooking 19 different dishes and ambient measurements at two Christmas markets measuring various particle properties and trace gases of emissions in real time. Similar emission characteristics were observed for dishes with the same preparation method, mainly due to similar cooking temperature and use of oil, with barbecuing as an especially strong source.
Michael Oluwatoyin Sunday, Laura Marie Dahler Heinlein, Junwei He, Allison Moon, Sukriti Kapur, Ting Fang, Kasey C. Edwards, Fangzhou Guo, Jack Dibb, James H. Flynn III, Becky Alexander, Manabu Shiraiwa, and Cort Anastasio
EGUsphere, https://doi.org/10.5194/egusphere-2024-3272, https://doi.org/10.5194/egusphere-2024-3272, 2024
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Hydrogen peroxide (HOOH) is an important oxidant that forms atmospheric sulfate. We demonstrate that illumination of brown carbon can rapidly form HOOH within particles, even under the low sunlight conditions of Fairbanks, Alaska during winter. This in-particle formation of HOOH is fast enough that it forms sulfate at significant rates. In contrast, the formation of HOOH in the gas phase during the campaign is expected to be negligible because of high NOx levels.
Yueyao Yang, Yahui Liu, Guohua Zhu, Bingcheng Lin, Shanshan Zhang, Xin Li, Fangxi Xu, He Niu, Rong Jin, and Minghui Zheng
EGUsphere, https://doi.org/10.5194/egusphere-2024-2814, https://doi.org/10.5194/egusphere-2024-2814, 2024
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Halogenated polycyclic aromatic hydrocarbons (XPAHs) are emerging pollutants. The stability during the atmospheric transformation processes is crucial for predicting their environmental fate and assessing associated risks. Here, we conducted field studies and laboratory simulation experiments to reveal the mechanisms, influencing factors and products for XPAHs’ heterogeneous phototransformation. Results revealed that the conversion of XPAHs led to a reduction in environmental risk.
Han Zang, Zekun Luo, Chenxi Li, Ziyue Li, Dandan Huang, and Yue Zhao
Atmos. Chem. Phys., 24, 11701–11716, https://doi.org/10.5194/acp-24-11701-2024, https://doi.org/10.5194/acp-24-11701-2024, 2024
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Atmospheric organics are subject to synergistic oxidation by different oxidants, yet the mechanisms of such processes are poorly understood. Here, using direct measurements and kinetic modeling, we probe the nocturnal synergistic-oxidation mechanism of α-pinene by O3 and NO3 radicals and in particular the fate of peroxy radical intermediates of different origins, which will deepen our understanding of the monoterpene oxidation chemistry and its contribution to atmospheric particle formation.
Hui Yang, Fengfeng Dong, Li Xia, Qishen Huang, Shufeng Pang, and Yunhong Zhang
Atmos. Chem. Phys., 24, 11619–11635, https://doi.org/10.5194/acp-24-11619-2024, https://doi.org/10.5194/acp-24-11619-2024, 2024
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Atmospheric secondary aerosols, composed of organic and inorganic components, undergo complex reactions that impact their phase state. Using molecular spectroscopy, we showed that ammonium-promoted aqueous replacement reaction, unique to these aerosols, is closely linked to phase behavior. The interplay between reactions and aerosol phase state can cause atypical phase transition and irreversible changes in aerosol composition during hygroscopic cycles, further impacting atmospheric processes.
Xiaoli Shen, David M. Bell, Hugh Coe, Naruki Hiranuma, Fabian Mahrt, Nicholas A. Marsden, Claudia Mohr, Daniel M. Murphy, Harald Saathoff, Johannes Schneider, Jacqueline Wilson, Maria A. Zawadowicz, Alla Zelenyuk, Paul J. DeMott, Ottmar Möhler, and Daniel J. Cziczo
Atmos. Chem. Phys., 24, 10869–10891, https://doi.org/10.5194/acp-24-10869-2024, https://doi.org/10.5194/acp-24-10869-2024, 2024
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Single-particle mass spectrometry (SPMS) is commonly used to measure the chemical composition and mixing state of aerosol particles. Intercomparison of SPMS instruments was conducted. All instruments reported similar size ranges and common spectral features. The instrument-specific detection efficiency was found to be more dependent on particle size than type. All differentiated secondary organic aerosol, soot, and soil dust but had difficulties differentiating among minerals and dusts.
Rhianna Louise Evans, Daniel Jack Bryant, Aristeidis Voliotis, Dawei Hu, Huihui Wu, Sara Aisyah Syafira, Osayomwanbor Ebenezer Oghama, Gordon McFiggans, Jacqueline Fiona Hamilton, and Andrew Robert Rickard
EGUsphere, https://doi.org/10.5194/egusphere-2024-2642, https://doi.org/10.5194/egusphere-2024-2642, 2024
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The chemical composition of organic aerosol derived from wood burning emissions under different burning conditions was characterised. Fresh emissions from flaming and smouldering were largely aromatic in nature whereas upon aging the aromatic content decreased. This decrease was greater for smouldering due to the loss of toxic polyaromatic species. Whereas under flaming conditions highly toxic polyaromatic species were produced. These differences present an important challenge for policy.
Adolfo González-Romero, Cristina González-Flórez, Agnesh Panta, Jesús Yus-Díez, Patricia Córdoba, Andres Alastuey, Natalia Moreno, Melani Hernández-Chiriboga, Konrad Kandler, Martina Klose, Roger N. Clark, Bethany L. Ehlmann, Rebecca N. Greenberger, Abigail M. Keebler, Phil Brodrick, Robert Green, Paul Ginoux, Xavier Querol, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 9155–9176, https://doi.org/10.5194/acp-24-9155-2024, https://doi.org/10.5194/acp-24-9155-2024, 2024
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In this research, we studied the dust-emitting properties of crusts and aeolian ripples from the Mojave Desert. These properties are key to understanding the effect of dust upon climate. We found two different playa lakes according to the groundwater regime, which implies differences in crusts' cohesion state and mineralogy, which can affect the dust emission potential and properties. We also compare them with Moroccan Sahara crusts and Icelandic top sediments.
Juanjuan Qin, Leiming Zhang, Yuanyuan Qin, Shaoxuan Shi, Jingnan Li, Zhao Shu, Yuwei Gao, Ting Qi, Jihua Tan, and Xinming Wang
Atmos. Chem. Phys., 24, 7575–7589, https://doi.org/10.5194/acp-24-7575-2024, https://doi.org/10.5194/acp-24-7575-2024, 2024
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The present research unveiled that acidity dominates while transition metal ions harmonize with the light absorption properties of humic-like substances (HULIS). Cu2+ has quenching effects on HULIS by complexation, hydrogen substitution, or electrostatic adsorption, with aromatic structures of HULIS. Such effects are less pronounced if from Mn2+, Ni2+, Zn2+, and Cu2+. Oxidized HULIS might contain electron-donating groups, whereas N-containing compounds might contain electron-withdrawing groups.
Adolfo González-Romero, Cristina González-Flórez, Agnesh Panta, Jesús Yus-Díez, Patricia Córdoba, Andres Alastuey, Natalia Moreno, Konrad Kandler, Martina Klose, Roger N. Clark, Bethany L. Ehlmann, Rebecca N. Greenberger, Abigail M. Keebler, Phil Brodrick, Robert O. Green, Xavier Querol, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 6883–6910, https://doi.org/10.5194/acp-24-6883-2024, https://doi.org/10.5194/acp-24-6883-2024, 2024
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The knowledge of properties from dust emitted in high latitudes such as in Iceland is scarce. This study focuses on the particle size, mineralogy, cohesion, and iron mode of occurrence and reflectance spectra of dust-emitting sediments. Icelandic top sediments have lower cohesion state, coarser particle size, distinctive mineralogy, and 3-fold bulk Fe content, with a large presence of magnetite compared to Saharan crusts.
Wangjin Yang, Jiawei Ma, Hongxing Yang, Fu Li, and Chong Han
Atmos. Chem. Phys., 24, 6757–6768, https://doi.org/10.5194/acp-24-6757-2024, https://doi.org/10.5194/acp-24-6757-2024, 2024
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We provide evidence that light enhances the conversion of SO2 to sulfates on non-photoactive mineral dust, where triplet states of SO2 (3SO2) can act as a pivotal trigger to generate sulfates. Photochemical sulfate formation depends on H2O, O2, and basicity of mineral dust. The SO2 photochemistry on non-photoactive mineral dust contributes to sulfates, highlighting previously unknown pathways to better explain the missing sources of atmospheric sulfates.
Lu Zhang, Jin Li, Yaojie Li, Xinlei Liu, Zhihan Luo, Guofeng Shen, and Shu Tao
Atmos. Chem. Phys., 24, 6323–6337, https://doi.org/10.5194/acp-24-6323-2024, https://doi.org/10.5194/acp-24-6323-2024, 2024
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Brown carbon (BrC) is related to radiative forcing and climate change. The BrC fraction from residential coal and biomass burning emissions, which were the major source of BrC, was characterized at the molecular level. The CHOS aromatic compounds explained higher light absorption efficiencies of biomass burning emissions compared to coal. The unique formulas of coal combustion aerosols were characterized by higher unsaturated compounds, and such information could be used for source appointment.
Wenli Liu, Longkun He, Yingjun Liu, Keren Liao, Qi Chen, and Mikinori Kuwata
Atmos. Chem. Phys., 24, 5625–5636, https://doi.org/10.5194/acp-24-5625-2024, https://doi.org/10.5194/acp-24-5625-2024, 2024
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Cooking is a major source of particles in urban areas. Previous studies demonstrated that the chemical lifetimes of cooking organic aerosols (COAs) were much shorter (~minutes) than the values reported by field observations (~hours). We conducted laboratory experiments to resolve the discrepancy by considering suppressed reactivity under low temperature. The parameterized k2–T relationships and observed surface temperature data were used to estimate the chemical lifetimes of COA particles.
Stephanie Arciva, Lan Ma, Camille Mavis, Chrystal Guzman, and Cort Anastasio
Atmos. Chem. Phys., 24, 4473–4485, https://doi.org/10.5194/acp-24-4473-2024, https://doi.org/10.5194/acp-24-4473-2024, 2024
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We measured changes in light absorption during the aqueous oxidation of six phenols with hydroxyl radical (●OH) or an organic triplet excited state (3C*). All the phenols formed light-absorbing secondary brown carbon (BrC), which then decayed with continued oxidation. Extrapolation to ambient conditions suggest ●OH is the dominant sink of secondary phenolic BrC in fog/cloud drops, while 3C* controls the lifetime of this light absorption in particle water.
Aaron Lieberman, Julietta Picco, Murat Onder, and Cort Anastasio
Atmos. Chem. Phys., 24, 4411–4419, https://doi.org/10.5194/acp-24-4411-2024, https://doi.org/10.5194/acp-24-4411-2024, 2024
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We developed a method that uses aqueous S(IV) to quantitatively convert NO2 to NO2−, which allows both species to be quantified using the Griess method. As an example of the utility of the method, we quantified both photolysis channels of nitrate, with and without a scavenger for hydroxyl radical (·OH). The results show that without a scavenger, ·OH reacts with nitrite to form nitrogen dioxide, suppressing the apparent quantum yield of NO2− and enhancing that of NO2.
Xingjun Fan, Ao Cheng, Xufang Yu, Tao Cao, Dan Chen, Wenchao Ji, Yongbing Cai, Fande Meng, Jianzhong Song, and Ping'an Peng
Atmos. Chem. Phys., 24, 3769–3783, https://doi.org/10.5194/acp-24-3769-2024, https://doi.org/10.5194/acp-24-3769-2024, 2024
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Molecular-level characteristics of high molecular weight (HMW) and low MW (LMW) humic-like substances (HULIS) were comprehensively investigated, where HMW HULIS had larger chromophores and larger molecular size than LMW HULIS and exhibited higher aromaticity and humification. Electrospray ionization high-resolution mass spectrometry revealed more aromatic molecules in HMW HULIS. HMW HULIS had more CHON compounds, while LMW HULIS had more CHO compounds.
Daniel A. Knopf, Markus Ammann, Thomas Berkemeier, Ulrich Pöschl, and Manabu Shiraiwa
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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The initial step of interfacial and multiphase chemical processes involves adsorption and desorption of gas species. This study demonstrates the role of desorption energy governing the residence time of the gas species at the environmental interface. A parameterization is formulated that enables the prediction of desorption energy based on the molecular weight, polarizability, and oxygen-to-carbon ratio of the desorbing chemical species. Its application to gas–particle interactions is discussed.
Feng Jiang, Kyla Siemens, Claudia Linke, Yanxia Li, Yiwei Gong, Thomas Leisner, Alexander Laskin, and Harald Saathoff
Atmos. Chem. Phys., 24, 2639–2649, https://doi.org/10.5194/acp-24-2639-2024, https://doi.org/10.5194/acp-24-2639-2024, 2024
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We investigated the optical properties, chemical composition, and formation mechanisms of secondary organic aerosol (SOA) and brown carbon (BrC) from the oxidation of indole with and without NO2 in the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) simulation chamber. This work is one of the very few to link the optical properties and chemical composition of indole SOA with and without NO2 by simulation chamber experiments.
Evangelia Kostenidou, Baptiste Marques, Brice Temime-Roussel, Yao Liu, Boris Vansevenant, Karine Sartelet, and Barbara D'Anna
Atmos. Chem. Phys., 24, 2705–2729, https://doi.org/10.5194/acp-24-2705-2024, https://doi.org/10.5194/acp-24-2705-2024, 2024
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Secondary organic aerosol (SOA) from gasoline vehicles can be a significant source of particulate matter in urban areas. Here the chemical composition of secondary volatile organic compounds and SOA produced by photo-oxidation of Euro 5 gasoline vehicle emissions was studied. The volatility of the SOA formed was calculated. Except for the temperature and the concentration of the aerosol, additional parameters may play a role in the gas-to-particle partitioning.
András Hoffer, Aida Meiramova, Ádám Tóth, Beatrix Jancsek-Turóczi, Gyula Kiss, Ágnes Rostási, Erika Andrea Levei, Luminita Marmureanu, Attila Machon, and András Gelencsér
Atmos. Chem. Phys., 24, 1659–1671, https://doi.org/10.5194/acp-24-1659-2024, https://doi.org/10.5194/acp-24-1659-2024, 2024
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Specific tracer compounds identified previously in controlled test burnings of different waste types in the laboratory were detected and quantified in ambient PM10 samples collected in five Hungarian and four Romanian settlements. Back-of-the-envelope calculations based on the relative emission factors of individual tracers suggested that the contribution of solid waste burning particulate emissions to ambient PM10 mass concentrations may be as high as a few percent.
Xiao-San Luo, Weijie Huang, Guofeng Shen, Yuting Pang, Mingwei Tang, Weijun Li, Zhen Zhao, Hanhan Li, Yaqian Wei, Longjiao Xie, and Tariq Mehmood
Atmos. Chem. Phys., 24, 1345–1360, https://doi.org/10.5194/acp-24-1345-2024, https://doi.org/10.5194/acp-24-1345-2024, 2024
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PM2.5 are air pollutants threatening health globally, but they are a mixture of chemical compositions from many sources and result in unequal toxicity. Which composition from which source of PM2.5 as the most hazardous object is a question hindering effective pollution control policy-making. With chemical and toxicity experiments, we found automobile exhaust and coal combustion to be priority emissions with higher toxic compositions for precise air pollution control, ensuring public health.
Matthew B. Goss and Jesse H. Kroll
Atmos. Chem. Phys., 24, 1299–1314, https://doi.org/10.5194/acp-24-1299-2024, https://doi.org/10.5194/acp-24-1299-2024, 2024
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The chemistry driving dimethyl sulfide (DMS) oxidation and subsequent sulfate particle formation in the atmosphere is poorly constrained. We oxidized two related compounds (dimethyl sulfoxide and dimethyl disulfide) in the laboratory under varied NOx conditions and measured the gas- and particle-phase products. These results demonstrate that both the OH addition and OH abstraction pathways for DMS oxidation contribute to particle formation via mechanisms that do not involve the SO2 intermediate.
Ryan J. Patnaude, Kathryn A. Moore, Russell J. Perkins, Thomas C. J. Hill, Paul J. DeMott, and Sonia M. Kreidenweis
Atmos. Chem. Phys., 24, 911–928, https://doi.org/10.5194/acp-24-911-2024, https://doi.org/10.5194/acp-24-911-2024, 2024
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In this study we examined the effect of atmospheric aging on sea spray aerosols (SSAs) to form ice and how newly formed secondary marine aerosols (SMAs) may freeze at cirrus temperatures (< −38 °C). Results show that SSAs freeze at different relative humidities (RHs) depending on the temperature and that the ice-nucleating ability of SSA was not hindered by atmospheric aging. SMAs are shown to freeze at high RHs and are likely inefficient at forming ice at cirrus temperatures.
Bartłomiej Witkowski, Priyanka Jain, Beata Wileńska, and Tomasz Gierczak
Atmos. Chem. Phys., 24, 663–688, https://doi.org/10.5194/acp-24-663-2024, https://doi.org/10.5194/acp-24-663-2024, 2024
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This article reports the results of the kinetic measurements for the aqueous oxidation of the 29 aliphatic alcohols by hydroxyl radical (OH) at different temperatures. The data acquired and the literature data were used to optimize a model for predicting the aqueous OH reactivity of alcohols and carboxylic acids and to estimate the atmospheric lifetimes of five terpenoic alcohols. The kinetic data provided new insights into the mechanism of aqueous oxidation of aliphatic molecules by the OH.
Junting Qiu, Xinlin Shen, Jiangyao Chen, Guiying Li, and Taicheng An
Atmos. Chem. Phys., 24, 155–166, https://doi.org/10.5194/acp-24-155-2024, https://doi.org/10.5194/acp-24-155-2024, 2024
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We studied reactions of secondary ozonides (SOZs) with amines. SOZs formed from ozonolysis of β-caryophyllene and α-humulene are found to be reactive to ethylamine and methylamine. Products from SOZs with various conformations reacting with the same amine had different functional groups. Our findings indicate that interaction of SOZs with amines in the atmosphere is very complicated, which is potentially a hitherto unrecognized source of N-containing compound formation.
Lan Ma, Reed Worland, Laura Heinlein, Chrystal Guzman, Wenqing Jiang, Christopher Niedek, Keith J. Bein, Qi Zhang, and Cort Anastasio
Atmos. Chem. Phys., 24, 1–21, https://doi.org/10.5194/acp-24-1-2024, https://doi.org/10.5194/acp-24-1-2024, 2024
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We measured concentrations of three photooxidants – the hydroxyl radical, triplet excited states of organic carbon, and singlet molecular oxygen – in fine particles collected over a year. Concentrations are highest in extracts of fresh biomass burning particles, largely because they have the highest particle concentrations and highest light absorption. When normalized by light absorption, rates of formation for each oxidant are generally similar for the four particle types we observed.
Adolfo González-Romero, Cristina González-Flórez, Agnesh Panta, Jesús Yus-Díez, Cristina Reche, Patricia Córdoba, Natalia Moreno, Andres Alastuey, Konrad Kandler, Martina Klose, Clarissa Baldo, Roger N. Clark, Zongbo Shi, Xavier Querol, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 23, 15815–15834, https://doi.org/10.5194/acp-23-15815-2023, https://doi.org/10.5194/acp-23-15815-2023, 2023
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The effect of dust emitted from desertic surfaces upon climate and ecosystems depends on size and mineralogy, but data from soil mineral atlases of desert soils are scarce. We performed particle-size distribution, mineralogy, and Fe speciation in southern Morocco. Results show coarser particles with high quartz proportion are near the elevated areas, while in depressed areas, sizes are finer, and proportions of clays and nano-Fe oxides are higher. This difference is important for dust modelling.
Victor Lannuque, Barbara D'Anna, Evangelia Kostenidou, Florian Couvidat, Alvaro Martinez-Valiente, Philipp Eichler, Armin Wisthaler, Markus Müller, Brice Temime-Roussel, Richard Valorso, and Karine Sartelet
Atmos. Chem. Phys., 23, 15537–15560, https://doi.org/10.5194/acp-23-15537-2023, https://doi.org/10.5194/acp-23-15537-2023, 2023
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Large uncertainties remain in understanding secondary organic aerosol (SOA) formation from toluene oxidation. In this study, speciation measurements in gaseous and particulate phases were carried out, providing partitioning and volatility data on individual toluene SOA components at different temperatures. A new detailed oxidation mechanism was developed to improve modeled speciation, and effects of different processes involved in gas–particle partitioning at the molecular scale are explored.
Xiaoliang Wang, Hatef Firouzkouhi, Judith C. Chow, John G. Watson, Steven Sai Hang Ho, Warren Carter, and Alexandra S. M. De Vos
Atmos. Chem. Phys., 23, 15375–15393, https://doi.org/10.5194/acp-23-15375-2023, https://doi.org/10.5194/acp-23-15375-2023, 2023
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Open burning of municipal solid waste emits chemicals that are harmful to the environment. This paper reports source profiles and emission factors for PM2.5 species and acidic/alkali gases from laboratory combustion of 10 waste categories (including plastics and biomass) that represent open burning in South Africa. Results will be useful for health and climate impact assessments, speciated emission inventories, source-oriented dispersion models, and receptor-based source apportionment.
Jun Zhang, Kun Li, Tiantian Wang, Erlend Gammelsæter, Rico K. Y. Cheung, Mihnea Surdu, Sophie Bogler, Deepika Bhattu, Dongyu S. Wang, Tianqu Cui, Lu Qi, Houssni Lamkaddam, Imad El Haddad, Jay G. Slowik, Andre S. H. Prevot, and David M. Bell
Atmos. Chem. Phys., 23, 14561–14576, https://doi.org/10.5194/acp-23-14561-2023, https://doi.org/10.5194/acp-23-14561-2023, 2023
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We conducted burning experiments to simulate various types of solid fuel combustion, including residential burning, wildfires, agricultural burning, cow dung, and plastic bag burning. The chemical composition of the particles was characterized using mass spectrometers, and new potential markers for different fuels were identified using statistical analysis. This work improves our understanding of emissions from solid fuel burning and offers support for refined source apportionment.
Hyun Gu Kang, Yanfang Chen, Yoojin Park, Thomas Berkemeier, and Hwajin Kim
Atmos. Chem. Phys., 23, 14307–14323, https://doi.org/10.5194/acp-23-14307-2023, https://doi.org/10.5194/acp-23-14307-2023, 2023
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D5 is an emerging anthropogenic pollutant that is ubiquitous in indoor and urban environments, and the OH oxidation of D5 forms secondary organosiloxane aerosol (SOSiA). Application of a kinetic box model that uses a volatility basis set (VBS) showed that consideration of oxidative aging (aging-VBS) predicts SOSiA formation much better than using a standard-VBS model. Ageing-dependent parameterization is needed to accurately model SOSiA to assess the implications of siloxanes for air quality.
Kai Song, Rongzhi Tang, Jingshun Zhang, Zichao Wan, Yuan Zhang, Kun Hu, Yuanzheng Gong, Daqi Lv, Sihua Lu, Yu Tan, Ruifeng Zhang, Ang Li, Shuyuan Yan, Shichao Yan, Baoming Fan, Wenfei Zhu, Chak K. Chan, Maosheng Yao, and Song Guo
Atmos. Chem. Phys., 23, 13585–13595, https://doi.org/10.5194/acp-23-13585-2023, https://doi.org/10.5194/acp-23-13585-2023, 2023
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Incense burning is common in Asia, posing threats to human health and air quality. However, less is known about its emissions and health risks. Full-volatility organic species from incense-burning smoke are detected and quantified. Intermediate-volatility volatile organic compounds (IVOCs) are crucial organics accounting for 19.2 % of the total emission factors (EFs) and 40.0 % of the secondary organic aerosol (SOA) estimation, highlighting the importance of incorporating IVOCs into SOA models.
Qianqian Gao, Shengqiang Zhu, Kaili Zhou, Jinghao Zhai, Shaodong Chen, Qihuang Wang, Shurong Wang, Jin Han, Xiaohui Lu, Hong Chen, Liwu Zhang, Lin Wang, Zimeng Wang, Xin Yang, Qi Ying, Hongliang Zhang, Jianmin Chen, and Xiaofei Wang
Atmos. Chem. Phys., 23, 13049–13060, https://doi.org/10.5194/acp-23-13049-2023, https://doi.org/10.5194/acp-23-13049-2023, 2023
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Dust is a major source of atmospheric aerosols. Its chemical composition is often assumed to be similar to the parent soil. However, this assumption has not been rigorously verified. Dust aerosols are mainly generated by wind erosion, which may have some chemical selectivity. Mn, Cd and Pb were found to be highly enriched in fine-dust (PM2.5) aerosols. In addition, estimation of heavy metal emissions from dust generation by air quality models may have errors without using proper dust profiles.
Daniel C. O. Thornton, Sarah D. Brooks, Elise K. Wilbourn, Jessica Mirrielees, Alyssa N. Alsante, Gerardo Gold-Bouchot, Andrew Whitesell, and Kiana McFadden
Atmos. Chem. Phys., 23, 12707–12729, https://doi.org/10.5194/acp-23-12707-2023, https://doi.org/10.5194/acp-23-12707-2023, 2023
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A major uncertainty in our understanding of clouds and climate is the sources and properties of the aerosol on which clouds grow. We found that aerosol containing organic matter from fast-growing marine phytoplankton was a source of ice-nucleating particles (INPs). INPs facilitate freezing of ice crystals at warmer temperatures than otherwise possible and therefore change cloud formation and properties. Our results show that ecosystem processes and the properties of sea spray aerosol are linked.
Adam Milsom, Shaojun Qi, Ashmi Mishra, Thomas Berkemeier, Zhenyu Zhang, and Christian Pfrang
Atmos. Chem. Phys., 23, 10835–10843, https://doi.org/10.5194/acp-23-10835-2023, https://doi.org/10.5194/acp-23-10835-2023, 2023
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Aerosols and films are found indoors and outdoors. Our study measures and models reactions of a cooking aerosol proxy with the atmospheric oxidant ozone relying on a low-cost but sensitive technique based on mass changes and film rigidity. We found that film morphology changed and film rigidity increased with evidence of surface crust formation during ozone exposure. Our modelling results demonstrate clear potential to take this robust method to the field for reaction monitoring.
Shan Zhang, Lin Du, Zhaomin Yang, Narcisse Tsona Tchinda, Jianlong Li, and Kun Li
Atmos. Chem. Phys., 23, 10809–10822, https://doi.org/10.5194/acp-23-10809-2023, https://doi.org/10.5194/acp-23-10809-2023, 2023
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In this study, we have investigated the distinct impacts of humidity on the ozonolysis of two structurally different monoterpenes (limonene and Δ3-carene). We found that the molecular structure of precursors can largely influence the SOA formation under high RH by impacting the multi-generation reactions. Our results could advance knowledge on the roles of water content in aerosol formation and inform ongoing research on particle environmental effects and applications in models.
Yangzhihao Zhan, Min Xie, Wei Zhao, Tijian Wang, Da Gao, Pulong Chen, Jun Tian, Kuanguang Zhu, Shu Li, Bingliang Zhuang, Mengmeng Li, Yi Luo, and Runqi Zhao
Atmos. Chem. Phys., 23, 9837–9852, https://doi.org/10.5194/acp-23-9837-2023, https://doi.org/10.5194/acp-23-9837-2023, 2023
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Although the main source contribution of pollution is secondary inorganic aerosols in Nanjing, health risks mainly come from industry sources and vehicle emissions. Therefore, the development of megacities should pay more attention to the health burden of vehicle emissions, coal combustion, and industrial processes. This study provides new insight into assessing the relationship between source apportionment and health risks and can provide valuable insight into air pollution strategies.
Jonathan P. D. Abbatt and A. R. Ravishankara
Atmos. Chem. Phys., 23, 9765–9785, https://doi.org/10.5194/acp-23-9765-2023, https://doi.org/10.5194/acp-23-9765-2023, 2023
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With important climate and air quality impacts, atmospheric multiphase chemistry involves gas interactions with aerosol particles and cloud droplets. We summarize the status of the field and discuss potential directions for future growth. We highlight the importance of a molecular-level understanding of the chemistry, along with atmospheric field studies and modeling, and emphasize the necessity for atmospheric multiphase chemists to interact widely with scientists from neighboring disciplines.
Zhancong Liang, Zhihao Cheng, Ruifeng Zhang, Yiming Qin, and Chak K. Chan
Atmos. Chem. Phys., 23, 9585–9595, https://doi.org/10.5194/acp-23-9585-2023, https://doi.org/10.5194/acp-23-9585-2023, 2023
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In this study, we found that the photolysis of sodium nitrate leads to a much quicker decay of free amino acids (FAAs, with glycine as an example) in the particle phase than ammonium nitrate photolysis, which is likely due to the molecular interactions between FAAs and different nitrate salts. Since sodium nitrate likely co-exists with FAAs in the coarse-mode particles, particulate nitrate photolysis can possibly contribute to a rapid decay of FAAs and affect atmospheric nitrogen cycling.
Julian Resch, Kate Wolfer, Alexandre Barth, and Markus Kalberer
Atmos. Chem. Phys., 23, 9161–9171, https://doi.org/10.5194/acp-23-9161-2023, https://doi.org/10.5194/acp-23-9161-2023, 2023
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Detailed chemical analysis of organic aerosols is necessary to better understand their effects on climate and health. Aerosol samples are often stored for days to months before analysis. We examined the effects of storage conditions (i.e., time, temperature, and aerosol storage on filters or as solvent extracts) on composition and found significant changes in the concentration of individual compounds, indicating that sample storage can strongly affect the detailed chemical particle composition.
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