Articles | Volume 16, issue 4
https://doi.org/10.5194/acp-16-2083-2016
© Author(s) 2016. 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-16-2083-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Analysis of isothermal and cooling-rate-dependent immersion freezing by a unifying stochastic ice nucleation model
Peter A. Alpert
CORRESPONDING AUTHOR
Institute for Terrestrial and Planetary Atmospheres/School of
Marine and Atmospheric Sciences, Stony Brook University, Stony Brook,
NY 11794-5000, USA
now at: Institut de Recherches sur la Catalyse
et l'Environnement de Lyon, Centre National de la Recherche Scientifique,
Université Claude Bernard Lyon 1, 69626 Villeurbanne, France
Daniel A. Knopf
CORRESPONDING AUTHOR
Institute for Terrestrial and Planetary Atmospheres/School of
Marine and Atmospheric Sciences, Stony Brook University, Stony Brook,
NY 11794-5000, USA
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This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Aerosol particles composed of metal complexes generate radicals as the result of photochemical reactions. Reactive species generated are hazardous to human health. We report microscopy data with particles composed of an organic proxy exposed to UV light. We found that copper influenced the reoxidation and initial iron reduction via photolysis of the complex. New model results suggest that we need to account a decreased photochemical activity and use a copper-induced reoxidation reaction.
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
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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.
Jing Dou, Peter A. Alpert, Pablo Corral Arroyo, Beiping Luo, Frederic Schneider, Jacinta Xto, Thomas Huthwelker, Camelia N. Borca, Katja D. Henzler, Jörg Raabe, Benjamin Watts, Hartmut Herrmann, Thomas Peter, Markus Ammann, and Ulrich K. Krieger
Atmos. Chem. Phys., 21, 315–338, https://doi.org/10.5194/acp-21-315-2021, https://doi.org/10.5194/acp-21-315-2021, 2021
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Photochemistry of iron(III) complexes plays an important role in aerosol aging, especially in the lower troposphere. Ensuing radical chemistry leads to decarboxylation, and the production of peroxides, and oxygenated volatile compounds, resulting in particle mass loss due to release of the volatile products to the gas phase. We investigated kinetic transport limitations due to high particle viscosity under low relative humidity conditions. For quantification a numerical model was developed.
Jan-David Förster, Christian Gurk, Mark Lamneck, Haijie Tong, Florian Ditas, Sarah S. Steimer, Peter A. Alpert, Markus Ammann, Jörg Raabe, Markus Weigand, Benjamin Watts, Ulrich Pöschl, Meinrat O. Andreae, and Christopher Pöhlker
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A gas flow system coupled with a microreactor for X-ray microspectroscopy is presented. Its core objective is to mimic the atmospheric processing of aerosol particles under laboratory conditions in a controlled gas-phase environment and allow in situ observations with high spatial and chemical resolution. We here emphasize its analytical capabilities and show initial results from hydration–dehydration experiments and the observation of water ice at low temperature and high relative humidity.
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Oxidation of bromide and iodide is an important process in the troposphere that leads to gas-phase halogen compounds which impact the oxidation capacity of the atmosphere. Imidazole-2-carboxaldehyde (IC), an aromatic carbonyl, is a product of the multiphase chemistry of glyoxal (an oxidation product of isoprene), a major biogenic volatile organic compound. In this study we demonstrate that IC photochemistry leads to efficient oxidation of bromide and iodide and liberation of halogen compounds.
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Atmospheric black carbon (BC), commonly known as soot, is an important constituent of the earth that imparts a warming similar to that of carbon dioxide. However, BC is much shorter lived and has uncertain warming due to its mixture with other solid and liquid components. Here, advanced microscopic methods have provided a detailed look at thousands of BC particles sampled from central California; these measurements will lead towards a better understanding of the effects that BC has on climate.
Y. J. Rigg, P. A. Alpert, and D. A. Knopf
Atmos. Chem. Phys., 13, 6603–6622, https://doi.org/10.5194/acp-13-6603-2013, https://doi.org/10.5194/acp-13-6603-2013, 2013
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EGUsphere, https://doi.org/10.5194/egusphere-2024-3226, https://doi.org/10.5194/egusphere-2024-3226, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Aerosol particles composed of metal complexes generate radicals as the result of photochemical reactions. Reactive species generated are hazardous to human health. We report microscopy data with particles composed of an organic proxy exposed to UV light. We found that copper influenced the reoxidation and initial iron reduction via photolysis of the complex. New model results suggest that we need to account a decreased photochemical activity and use a copper-induced reoxidation reaction.
Albert Ansmann, Cristofer Jimenez, Johanna Roschke, Johannes Bühl, Kevin Ohneiser, Ronny Engelmann, Martin Radenz, Hannes Griesche, Julian Hofer, Dietrich Althausen, Daniel A. Knopf, Sandro Dahlke, Tom Gaudek, Patric Seifert, and Ulla Wandinger
EGUsphere, https://doi.org/10.5194/egusphere-2024-2008, https://doi.org/10.5194/egusphere-2024-2008, 2024
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In this study, we focus on the potential impact of wildfire smoke on cirrus formation. For the first time, state-of-the-art aerosol and cirrus observations with lidar and radar, presented in part 1 of a series of two articles, are closely linked to comprehensive modeling of gravity-wave-induced ice nucleation in cirrus evolution processes, presented in part 2. We found a clear impact of wildfire smoke on cirrus evolution.
Albert Ansmann, Cristofer Jimenez, Daniel A. Knopf, Johanna Roschke, Johannes Bühl, Kevin Ohneiser, and Ronny Engelmann
EGUsphere, https://doi.org/10.5194/egusphere-2024-2009, https://doi.org/10.5194/egusphere-2024-2009, 2024
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In this study, we focus on the potential impact of wildfire smoke on cirrus formation. Aerosol and cirrus observations with lidar and radar during the MOSAiC expedition, presented in part 1 (egusphere-2024-2008) are closely linked to comprehensive modeling of ice nucleation in cirrus evolution processes, presented in this part 2 (egusphere-2024-2009). A clear impact of wildfire smoke on cirrus formation was found.
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.
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.
Rodanthi-Elisavet Mamouri, Albert Ansmann, Kevin Ohneiser, Daniel A. Knopf, Argyro Nisantzi, Johannes Bühl, Ronny Engelmann, Annett Skupin, Patric Seifert, Holger Baars, Dragos Ene, Ulla Wandinger, and Diofantos Hadjimitsis
Atmos. Chem. Phys., 23, 14097–14114, https://doi.org/10.5194/acp-23-14097-2023, https://doi.org/10.5194/acp-23-14097-2023, 2023
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For the first time, rather clear evidence is found that wildfire smoke particles can trigger strong cirrus formation. This finding is of importance because intensive and large wildfires may occur increasingly often in the future as climate change proceeds. Based on lidar observations in Cyprus in autumn 2020, we provide detailed insight into the cirrus formation at the tropopause in the presence of aged wildfire smoke (here, 8–9 day old Californian wildfire smoke).
Albert Ansmann, Kevin Ohneiser, Ronny Engelmann, Martin Radenz, Hannes Griesche, Julian Hofer, Dietrich Althausen, Jessie M. Creamean, Matthew C. Boyer, Daniel A. Knopf, Sandro Dahlke, Marion Maturilli, Henriette Gebauer, Johannes Bühl, Cristofer Jimenez, Patric Seifert, and Ulla Wandinger
Atmos. Chem. Phys., 23, 12821–12849, https://doi.org/10.5194/acp-23-12821-2023, https://doi.org/10.5194/acp-23-12821-2023, 2023
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The 1-year MOSAiC (2019–2020) expedition with the German ice breaker Polarstern was the largest polar field campaign ever conducted. The Polarstern, with our lidar aboard, drifted with the pack ice north of 85° N for more than 7 months (October 2019 to mid-May 2020). We measured the full annual cycle of aerosol conditions in terms of aerosol optical and cloud-process-relevant properties. We observed a strong contrast between polluted winter and clean summer aerosol conditions.
Daniel A. Knopf, Peiwen Wang, Benny Wong, Jay M. Tomlin, Daniel P. Veghte, Nurun N. Lata, Swarup China, Alexander Laskin, Ryan C. Moffet, Josephine Y. Aller, Matthew A. Marcus, and Jian Wang
Atmos. Chem. Phys., 23, 8659–8681, https://doi.org/10.5194/acp-23-8659-2023, https://doi.org/10.5194/acp-23-8659-2023, 2023
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Ambient particle populations and associated ice-nucleating particles (INPs)
were examined from particle samples collected on board aircraft in the marine
boundary layer and free troposphere in the eastern North Atlantic during
summer and winter. Chemical imaging shows distinct differences in the
particle populations seasonally and with sampling altitudes, which are
reflected in the INP types. Freezing parameterizations are derived for
implementation in cloud-resolving and climate models.
Albert Ansmann, Kevin Ohneiser, Alexandra Chudnovsky, Daniel A. Knopf, Edwin W. Eloranta, Diego Villanueva, Patric Seifert, Martin Radenz, Boris Barja, Félix Zamorano, Cristofer Jimenez, Ronny Engelmann, Holger Baars, Hannes Griesche, Julian Hofer, Dietrich Althausen, and Ulla Wandinger
Atmos. Chem. Phys., 22, 11701–11726, https://doi.org/10.5194/acp-22-11701-2022, https://doi.org/10.5194/acp-22-11701-2022, 2022
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For the first time we present a systematic study on the impact of wildfire smoke on ozone depletion in the Arctic (2020) and Antarctic stratosphere (2020, 2021). Two major fire events in Siberia and Australia were responsible for the observed record-breaking stratospheric smoke pollution. Our analyses were based on lidar observations of smoke parameters (Polarstern, Punta Arenas) and NDACC Arctic and Antarctic ozone profiles as well as on Antarctic OMI satellite observations of column ozone.
Kevin Ohneiser, Albert Ansmann, Bernd Kaifler, Alexandra Chudnovsky, Boris Barja, Daniel A. Knopf, Natalie Kaifler, Holger Baars, Patric Seifert, Diego Villanueva, Cristofer Jimenez, Martin Radenz, Ronny Engelmann, Igor Veselovskii, and Félix Zamorano
Atmos. Chem. Phys., 22, 7417–7442, https://doi.org/10.5194/acp-22-7417-2022, https://doi.org/10.5194/acp-22-7417-2022, 2022
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We present and discuss 2 years of long-term lidar observations of the largest stratospheric perturbation by wildfire smoke ever observed. The smoke originated from the record-breaking Australian fires in 2019–2020 and affects climate conditions and even the ozone layer in the Southern Hemisphere. The obvious link between dense smoke occurrence in the stratosphere and strong ozone depletion found in the Arctic and in the Antarctic in 2020 can be regarded as a new aspect of climate change.
Daniel A. Knopf, Joseph C. Charnawskas, Peiwen Wang, Benny Wong, Jay M. Tomlin, Kevin A. Jankowski, Matthew Fraund, Daniel P. Veghte, Swarup China, Alexander Laskin, Ryan C. Moffet, Mary K. Gilles, Josephine Y. Aller, Matthew A. Marcus, Shira Raveh-Rubin, and Jian Wang
Atmos. Chem. Phys., 22, 5377–5398, https://doi.org/10.5194/acp-22-5377-2022, https://doi.org/10.5194/acp-22-5377-2022, 2022
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Marine boundary layer aerosols collected in the remote region of the eastern North Atlantic induce immersion freezing and deposition ice nucleation under typical mixed-phase and cirrus cloud conditions. Corresponding ice nucleation parameterizations for model applications have been derived. Chemical imaging of ambient aerosol and ice-nucleating particles demonstrates that the latter is dominated by sea salt and organics while also representing a major particle type in the particle population.
Jay M. Tomlin, Kevin A. Jankowski, Daniel P. Veghte, Swarup China, Peiwen Wang, Matthew Fraund, Johannes Weis, Guangjie Zheng, Yang Wang, Felipe Rivera-Adorno, Shira Raveh-Rubin, Daniel A. Knopf, Jian Wang, Mary K. Gilles, Ryan C. Moffet, and Alexander Laskin
Atmos. Chem. Phys., 21, 18123–18146, https://doi.org/10.5194/acp-21-18123-2021, https://doi.org/10.5194/acp-21-18123-2021, 2021
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Analysis of individual atmospheric particles shows that aerosol transported from North America during meteorological dry intrusion episodes may have a substantial impact on the mixing state and particle-type population over the mid-Atlantic, as organic contribution and particle-type diversity are significantly enhanced during these periods. These observations need to be considered in current atmospheric models.
Daniel A. Knopf and Markus Ammann
Atmos. Chem. Phys., 21, 15725–15753, https://doi.org/10.5194/acp-21-15725-2021, https://doi.org/10.5194/acp-21-15725-2021, 2021
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Adsorption on and desorption of gas molecules from solid or liquid surfaces or interfaces represent the initial interaction of gas-to-condensed-phase processes that can define the physicochemical evolution of the condensed phase. We apply a thermodynamic and microscopic treatment of these multiphase processes to evaluate how adsorption and desorption rates and surface accommodation depend on the choice of adsorption model and standard states with implications for desorption energy and lifetimes.
Yang Wang, Guangjie Zheng, Michael P. Jensen, Daniel A. Knopf, Alexander Laskin, Alyssa A. Matthews, David Mechem, Fan Mei, Ryan Moffet, Arthur J. Sedlacek, John E. Shilling, Stephen Springston, Amy Sullivan, Jason Tomlinson, Daniel Veghte, Rodney Weber, Robert Wood, Maria A. Zawadowicz, and Jian Wang
Atmos. Chem. Phys., 21, 11079–11098, https://doi.org/10.5194/acp-21-11079-2021, https://doi.org/10.5194/acp-21-11079-2021, 2021
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This paper reports the vertical profiles of trace gas and aerosol properties over the eastern North Atlantic, a region of persistent but diverse subtropical marine boundary layer (MBL) clouds. We examined the key processes that drive the cloud condensation nuclei (CCN) population and how it varies with season and synoptic conditions. This study helps improve the model representation of the aerosol processes in the remote MBL, reducing the simulated aerosol indirect effects.
Albert Ansmann, Kevin Ohneiser, Rodanthi-Elisavet Mamouri, Daniel A. Knopf, Igor Veselovskii, Holger Baars, Ronny Engelmann, Andreas Foth, Cristofer Jimenez, Patric Seifert, and Boris Barja
Atmos. Chem. Phys., 21, 9779–9807, https://doi.org/10.5194/acp-21-9779-2021, https://doi.org/10.5194/acp-21-9779-2021, 2021
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We present retrievals of tropospheric and stratospheric height profiles of particle mass, volume, surface area concentration of wildfire smoke layers, and related cloud condensation nuclei (CCN) and ice-nucleating particle (INP) concentrations. The new analysis scheme is applied to ground-based lidar observations of stratospheric Australian smoke over southern South America and to spaceborne lidar observations of tropospheric North American smoke.
Alexander Zaytsev, Martin Breitenlechner, Anna Novelli, Hendrik Fuchs, Daniel A. Knopf, Jesse H. Kroll, and Frank N. Keutsch
Atmos. Meas. Tech., 14, 2501–2513, https://doi.org/10.5194/amt-14-2501-2021, https://doi.org/10.5194/amt-14-2501-2021, 2021
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We have developed an online method for speciated measurements of organic peroxy radicals and stabilized Criegee intermediates using chemical derivatization combined with chemical ionization mass spectrometry. Chemical derivatization prevents secondary radical reactions and eliminates potential interferences. Comparison between our measurements and results from numeric modeling shows that the method can be used for the quantification of a wide range of atmospheric radicals and intermediates.
Israel Silber, Ann M. Fridlind, Johannes Verlinde, Andrew S. Ackerman, Grégory V. Cesana, and Daniel A. Knopf
Atmos. Chem. Phys., 21, 3949–3971, https://doi.org/10.5194/acp-21-3949-2021, https://doi.org/10.5194/acp-21-3949-2021, 2021
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Long-term ground-based radar and sounding measurements over Alaska (Antarctica) indicate that more than 85 % (75 %) of supercooled clouds are precipitating at cloud base and that 75 % (50 %) are precipitating to the surface. Such high prevalence is reconciled with lesser spaceborne estimates by considering radar sensitivity. Results provide a strong observational constraint for polar cloud processes in large-scale models.
Jing Dou, Peter A. Alpert, Pablo Corral Arroyo, Beiping Luo, Frederic Schneider, Jacinta Xto, Thomas Huthwelker, Camelia N. Borca, Katja D. Henzler, Jörg Raabe, Benjamin Watts, Hartmut Herrmann, Thomas Peter, Markus Ammann, and Ulrich K. Krieger
Atmos. Chem. Phys., 21, 315–338, https://doi.org/10.5194/acp-21-315-2021, https://doi.org/10.5194/acp-21-315-2021, 2021
Short summary
Short summary
Photochemistry of iron(III) complexes plays an important role in aerosol aging, especially in the lower troposphere. Ensuing radical chemistry leads to decarboxylation, and the production of peroxides, and oxygenated volatile compounds, resulting in particle mass loss due to release of the volatile products to the gas phase. We investigated kinetic transport limitations due to high particle viscosity under low relative humidity conditions. For quantification a numerical model was developed.
Jan-David Förster, Christian Gurk, Mark Lamneck, Haijie Tong, Florian Ditas, Sarah S. Steimer, Peter A. Alpert, Markus Ammann, Jörg Raabe, Markus Weigand, Benjamin Watts, Ulrich Pöschl, Meinrat O. Andreae, and Christopher Pöhlker
Atmos. Meas. Tech., 13, 3717–3729, https://doi.org/10.5194/amt-13-3717-2020, https://doi.org/10.5194/amt-13-3717-2020, 2020
Short summary
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A gas flow system coupled with a microreactor for X-ray microspectroscopy is presented. Its core objective is to mimic the atmospheric processing of aerosol particles under laboratory conditions in a controlled gas-phase environment and allow in situ observations with high spatial and chemical resolution. We here emphasize its analytical capabilities and show initial results from hydration–dehydration experiments and the observation of water ice at low temperature and high relative humidity.
Jienan Li, Seanna M. Forrester, and Daniel A. Knopf
Atmos. Chem. Phys., 20, 6055–6080, https://doi.org/10.5194/acp-20-6055-2020, https://doi.org/10.5194/acp-20-6055-2020, 2020
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Organic aerosol is ubiquitous in the atmosphere and can change its phase state from liquid to solid in response to temperature. Our laboratory measurements demonstrate that the chemical reactivity of typical organic aerosol species with atmospheric oxidants is modulated by the species’ phase state. We find that under temperatures typical of the middle and upper troposphere the chemical lifetime of organic aerosol can be significantly extended due to the reduced reactive uptake of gas oxidants.
Pablo Corral Arroyo, Raffael Aellig, Peter A. Alpert, Rainer Volkamer, and Markus Ammann
Atmos. Chem. Phys., 19, 10817–10828, https://doi.org/10.5194/acp-19-10817-2019, https://doi.org/10.5194/acp-19-10817-2019, 2019
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Oxidation of bromide and iodide is an important process in the troposphere that leads to gas-phase halogen compounds which impact the oxidation capacity of the atmosphere. Imidazole-2-carboxaldehyde (IC), an aromatic carbonyl, is a product of the multiphase chemistry of glyoxal (an oxidation product of isoprene), a major biogenic volatile organic compound. In this study we demonstrate that IC photochemistry leads to efficient oxidation of bromide and iodide and liberation of halogen compounds.
Ryan C. Moffet, Rachel E. O'Brien, Peter A. Alpert, Stephen T. Kelly, Don Q. Pham, Mary K. Gilles, Daniel A. Knopf, and Alexander Laskin
Atmos. Chem. Phys., 16, 14515–14525, https://doi.org/10.5194/acp-16-14515-2016, https://doi.org/10.5194/acp-16-14515-2016, 2016
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Atmospheric black carbon (BC), commonly known as soot, is an important constituent of the earth that imparts a warming similar to that of carbon dioxide. However, BC is much shorter lived and has uncertain warming due to its mixture with other solid and liquid components. Here, advanced microscopic methods have provided a detailed look at thousands of BC particles sampled from central California; these measurements will lead towards a better understanding of the effects that BC has on climate.
J. H. Slade, R. Thalman, J. Wang, and D. A. Knopf
Atmos. Chem. Phys., 15, 10183–10201, https://doi.org/10.5194/acp-15-10183-2015, https://doi.org/10.5194/acp-15-10183-2015, 2015
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Aerosol particles undergo chemical modification during atmospheric transport due to reactions with trace gas species such as OH radicals affecting cloud formation and, thus, prediction of climate. Here, the cloud formation potential of surrogate biomass burning aerosol (BBA) is studied as a function of particle composition and OH exposure. We find that OH oxidation can alter the cloud formation potential of BBA, but its significance depends on the available water-soluble particulate material.
Y. J. Rigg, P. A. Alpert, and D. A. Knopf
Atmos. Chem. Phys., 13, 6603–6622, https://doi.org/10.5194/acp-13-6603-2013, https://doi.org/10.5194/acp-13-6603-2013, 2013
S. M. Forrester and D. A. Knopf
Atmos. Chem. Phys., 13, 6507–6522, https://doi.org/10.5194/acp-13-6507-2013, https://doi.org/10.5194/acp-13-6507-2013, 2013
Related subject area
Subject: Clouds and Precipitation | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Physics (physical properties and processes)
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Jennifer R. Stout, Christopher D. Westbrook, Thorwald H. M. Stein, and Mark W. McCorquodale
Atmos. Chem. Phys., 24, 11133–11155, https://doi.org/10.5194/acp-24-11133-2024, https://doi.org/10.5194/acp-24-11133-2024, 2024
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This study uses 3D-printed ice crystal analogues falling in a water–glycerine mix and observed with multi-view cameras, simulating atmospheric conditions. Four types of motion are observed: stable, zigzag, transitional, and spiralling. Particle shape strongly influences motion; complex shapes have a wider range of conditions where they fall steadily compared to simple plates. The most common orientation of unstable particles is non-horizontal, contrary to prior assumptions of always horizontal.
Johanna S. Seidel, Alexei A. Kiselev, Alice Keinert, Frank Stratmann, Thomas Leisner, and Susan Hartmann
Atmos. Chem. Phys., 24, 5247–5263, https://doi.org/10.5194/acp-24-5247-2024, https://doi.org/10.5194/acp-24-5247-2024, 2024
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Clouds often contain several thousand times more ice crystals than aerosol particles catalyzing ice formation. This phenomenon, commonly known as ice multiplication, is often explained by secondary ice formation due to the collisions between falling ice particles and droplets. In this study, we mimic this riming process. Contrary to earlier experiments, we found no efficient ice multiplication, which fundamentally questions the importance of the rime-splintering mechanism.
Pierre Grzegorczyk, Sudha Yadav, Florian Zanger, Alexander Theis, Subir K. Mitra, Stephan Borrmann, and Miklós Szakáll
Atmos. Chem. Phys., 23, 13505–13521, https://doi.org/10.5194/acp-23-13505-2023, https://doi.org/10.5194/acp-23-13505-2023, 2023
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Secondary ice production generates high concentrations of ice crystals in clouds. These processes have been poorly understood. We conducted experiments at the wind tunnel laboratory of the Johannes Gutenberg University, Mainz, on graupel–graupel and graupel–snowflake collisions. From these experiments fragment number, size, cross-sectional area, and aspect ratio were determined.
Elise Rosky, Will Cantrell, Tianshu Li, Issei Nakamura, and Raymond A. Shaw
Atmos. Chem. Phys., 23, 10625–10642, https://doi.org/10.5194/acp-23-10625-2023, https://doi.org/10.5194/acp-23-10625-2023, 2023
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Using computer simulations of water, we find that water under tension freezes more easily than under normal conditions. A linear equation describes how freezing temperature increases with tension. Accordingly, simulations show that naturally occurring tension in water capillary bridges leads to higher freezing temperatures. This work is an early step in determining if atmospheric cloud droplets freeze due to naturally occurring tension, for example, during processes such as droplet collisions.
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.
Kara D. Lamb, Jerry Y. Harrington, Benjamin W. Clouser, Elisabeth J. Moyer, Laszlo Sarkozy, Volker Ebert, Ottmar Möhler, and Harald Saathoff
Atmos. Chem. Phys., 23, 6043–6064, https://doi.org/10.5194/acp-23-6043-2023, https://doi.org/10.5194/acp-23-6043-2023, 2023
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This study investigates how ice grows directly from vapor in cirrus clouds by comparing observations of populations of ice crystals growing in a cloud chamber against models developed in the context of single-crystal laboratory studies. We demonstrate that previous discrepancies between different experimental measurements do not necessarily point to different physical interpretations but are rather due to assumptions that were made in terms of how experiments were modeled in previous studies.
Anand Kumar, Kristian Klumpp, Chen Barak, Giora Rytwo, Michael Plötze, Thomas Peter, and Claudia Marcolli
Atmos. Chem. Phys., 23, 4881–4902, https://doi.org/10.5194/acp-23-4881-2023, https://doi.org/10.5194/acp-23-4881-2023, 2023
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Smectites are a major class of clay minerals that are ice nucleation (IN) active. They form platelets that swell or even delaminate in water by intercalation of water between their layers. We hypothesize that at least three smectite layers need to be stacked together to host a critical ice embryo on clay mineral edges and that the larger the surface edge area is, the higher the freezing temperature. Edge sites on such clay particles play a crucial role in imparting IN ability to such particles.
Chun-Ning Mao, Kanishk Gohil, and Akua A. Asa-Awuku
Atmos. Chem. Phys., 22, 13219–13228, https://doi.org/10.5194/acp-22-13219-2022, https://doi.org/10.5194/acp-22-13219-2022, 2022
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The impact of molecular-level surface chemistry for aerosol water uptake and droplet growth is not well understood. In this work we show changes in water uptake due to molecular-level surface chemistry can be measured and quantified. In addition, we develop a single-parameter model, representing changes in aerosol chemistry that can be used in global climate models to reduce the uncertainty in aerosol-cloud predictions.
Diana L. Pereira, Irma Gavilán, Consuelo Letechipía, Graciela B. Raga, Teresa Pi Puig, Violeta Mugica-Álvarez, Harry Alvarez-Ospina, Irma Rosas, Leticia Martinez, Eva Salinas, Erika T. Quintana, Daniel Rosas, and Luis A. Ladino
Atmos. Chem. Phys., 22, 6435–6447, https://doi.org/10.5194/acp-22-6435-2022, https://doi.org/10.5194/acp-22-6435-2022, 2022
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Airborne particles were i) collected in an agricultural fields and ii) generated in the laboratory from agricultural soil samples to analyze their ice nucleating abilities. It was found that the size and chemical composition of the Mexican agricultural dust particles influence their ice nucleating behavior, where the organic components are likely responsible for their efficiency as INPs. The INP concentrations from the present study are comparable to those from higher latitudes.
Kristian Klumpp, Claudia Marcolli, and Thomas Peter
Atmos. Chem. Phys., 22, 3655–3673, https://doi.org/10.5194/acp-22-3655-2022, https://doi.org/10.5194/acp-22-3655-2022, 2022
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Surface interactions with solutes can significantly alter the ice nucleation activity of mineral dust. Past studies revealed the sensitivity of microcline, one of the most ice-active types of dust in the atmosphere, to inorganic solutes. This study focuses on the interaction of microcline with bio-organic substances and the resulting effects on its ice nucleation activity. We observe strongly hampered ice nucleation activity due to the presence of carboxylic and amino acids but not for polyols.
Rachel L. James, Vaughan T. J. Phillips, and Paul J. Connolly
Atmos. Chem. Phys., 21, 18519–18530, https://doi.org/10.5194/acp-21-18519-2021, https://doi.org/10.5194/acp-21-18519-2021, 2021
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Secondary ice production (SIP) plays an important role in ice formation within mixed-phase clouds. We present a laboratory investigation of a potentially new SIP mechanism involving the collisions of supercooled water drops with ice particles. At impact, the supercooled water drop fragments form smaller secondary drops. Approximately 30 % of the secondary drops formed during the retraction phase of the supercooled water drop impact freeze over a temperature range of −4 °C to −12 °C.
Julia Schneider, Kristina Höhler, Robert Wagner, Harald Saathoff, Martin Schnaiter, Tobias Schorr, Isabelle Steinke, Stefan Benz, Manuel Baumgartner, Christian Rolf, Martina Krämer, Thomas Leisner, and Ottmar Möhler
Atmos. Chem. Phys., 21, 14403–14425, https://doi.org/10.5194/acp-21-14403-2021, https://doi.org/10.5194/acp-21-14403-2021, 2021
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Homogeneous freezing is a relevant mechanism for the formation of cirrus clouds in the upper troposphere. Based on an extensive set of homogeneous freezing experiments at the AIDA chamber with aqueous sulfuric acid aerosol, we provide a new fit line for homogeneous freezing onset conditions of sulfuric acid aerosol focusing on cirrus temperatures. In the atmosphere, homogeneous freezing thresholds have important implications on the cirrus cloud occurrence and related cloud radiative effects.
Naruki Hiranuma, Brent W. Auvermann, Franco Belosi, Jack Bush, Kimberly M. Cory, Dimitrios G. Georgakopoulos, Kristina Höhler, Yidi Hou, Larissa Lacher, Harald Saathoff, Gianni Santachiara, Xiaoli Shen, Isabelle Steinke, Romy Ullrich, Nsikanabasi S. Umo, Hemanth S. K. Vepuri, Franziska Vogel, and Ottmar Möhler
Atmos. Chem. Phys., 21, 14215–14234, https://doi.org/10.5194/acp-21-14215-2021, https://doi.org/10.5194/acp-21-14215-2021, 2021
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We present laboratory and field studies showing that an open-lot livestock facility is a substantial source of atmospheric ice-nucleating particles (INPs). The ambient concentration of INPs from livestock facilities in Texas is very high. It is up to several thousand INPs per liter below –20 °C and may impact regional aerosol–cloud interactions. About 50% of feedlot INPs were supermicron in diameter. No notable amount of known ice-nucleating microorganisms was found in our feedlot samples.
Vaughan T. J. Phillips, Jun-Ichi Yano, Akash Deshmukh, and Deepak Waman
Atmos. Chem. Phys., 21, 11941–11953, https://doi.org/10.5194/acp-21-11941-2021, https://doi.org/10.5194/acp-21-11941-2021, 2021
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For decades, high concentrations of ice observed in precipitating mixed-phase clouds have created an enigma. Such concentrations are higher than can be explained by the action of aerosols or by the spontaneous freezing of most cloud droplets. The controversy has partly persisted due to the lack of laboratory experimentation in ice microphysics, especially regarding fragmentation of ice, a topic reviewed by a recent paper. Our comment attempts to clarify some issues with regards to that review.
Alexei A. Kiselev, Alice Keinert, Tilia Gaedeke, Thomas Leisner, Christoph Sutter, Elena Petrishcheva, and Rainer Abart
Atmos. Chem. Phys., 21, 11801–11814, https://doi.org/10.5194/acp-21-11801-2021, https://doi.org/10.5194/acp-21-11801-2021, 2021
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Alkali feldspar is the most abundant mineral in the Earth's crust and is often present in mineral dust aerosols that are responsible for the formation of rain and snow in clouds. However, the cloud droplets containing pure potassium-rich feldspar would not freeze unless cooled down to a very low temperature. Here we show that partly replacing potassium with sodium would induce fracturing of feldspar, exposing a crystalline surface that could initiate freezing at higher temperature.
Barbara Bertozzi, Robert Wagner, Junwei Song, Kristina Höhler, Joschka Pfeifer, Harald Saathoff, Thomas Leisner, and Ottmar Möhler
Atmos. Chem. Phys., 21, 10779–10798, https://doi.org/10.5194/acp-21-10779-2021, https://doi.org/10.5194/acp-21-10779-2021, 2021
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Internally mixed particles composed of sulfate and organics are among the most abundant aerosol types. Their ice nucleation (IN) ability influences the formation of cirrus and, thus, the climate. We show that the presence of a thin organic coating suppresses the heterogeneous IN ability of crystalline ammonium sulfate particles. However, the IN ability of the same particle can substantially change if subjected to atmospheric processing, mainly due to differences in the resulting morphology.
Hemanth S. K. Vepuri, Cheyanne A. Rodriguez, Dimitrios G. Georgakopoulos, Dustin Hume, James Webb, Gregory D. Mayer, and Naruki Hiranuma
Atmos. Chem. Phys., 21, 4503–4520, https://doi.org/10.5194/acp-21-4503-2021, https://doi.org/10.5194/acp-21-4503-2021, 2021
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Due to a high frequency of storm events, West Texas is an ideal location to study ice-nucleating particles (INPs) in severe precipitation. Our results present that cumulative INP concentration in our precipitation samples below −20 °C could be high in the samples collected while observing > 10 mm h−1 precipitation with notably large hydrometeor sizes and an implication of cattle feedyard bacteria inclusion. Marine bacteria were found in a subset of our precipitation and cattle feedyard samples.
Miklós Szakáll, Michael Debertshäuser, Christian Philipp Lackner, Amelie Mayer, Oliver Eppers, Karoline Diehl, Alexander Theis, Subir Kumar Mitra, and Stephan Borrmann
Atmos. Chem. Phys., 21, 3289–3316, https://doi.org/10.5194/acp-21-3289-2021, https://doi.org/10.5194/acp-21-3289-2021, 2021
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The freezing of cloud drops is promoted by ice-nucleating particles immersed in the drops. This process is essential to understand ice and subsequent precipitation formation in clouds. We investigated the efficiency of several particle types to trigger immersion freezing with two single-drop levitation techniques: a wind tunnel and an acoustic levitator. The evaluation accounted for different conditions during our two series of experiments, which is also applicable to future comparison studies.
Gabor Vali
Atmos. Chem. Phys., 21, 2551–2568, https://doi.org/10.5194/acp-21-2551-2021, https://doi.org/10.5194/acp-21-2551-2021, 2021
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The freezing of water drops in clouds is a prime example for the role of ice-nucleating particles (INPs). Mercuric iodide particles and a few other substances can be conditioned to become very effective INPs after previous ice formation and moderate heating to melt temperatures, opening a new pathway to ice formation in the atmosphere and in other systems like tissue preservation, artificial snow making, and more.
Maximilian Weitzel, Subir K. Mitra, Miklós Szakáll, Jacob P. Fugal, and Stephan Borrmann
Atmos. Chem. Phys., 20, 14889–14901, https://doi.org/10.5194/acp-20-14889-2020, https://doi.org/10.5194/acp-20-14889-2020, 2020
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The properties of ice crystals smaller than 150 µm in diameter were investigated in a cold-room laboratory using digital holography and microscopy. Automated image processing has been used to determine the track of falling ice crystals, and collected crystals were melted and scanned under a microscope to infer particle mass. A parameterization relating particle size and mass was determined which describes ice crystals in this size range more accurately than existing relationships.
Alexei Korolev and Thomas Leisner
Atmos. Chem. Phys., 20, 11767–11797, https://doi.org/10.5194/acp-20-11767-2020, https://doi.org/10.5194/acp-20-11767-2020, 2020
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Secondary ice production (SIP) plays a key role in the formation of ice particles in tropospheric clouds. This work presents a critical review of the laboratory studies related to secondary ice production. It aims to identify gaps in our knowledge of SIP as well as to stimulate further laboratory studies focused on obtaining a quantitative description of efficiencies for each SIP mechanism.
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.
Steven K. Krueger
Atmos. Chem. Phys., 20, 7895–7909, https://doi.org/10.5194/acp-20-7895-2020, https://doi.org/10.5194/acp-20-7895-2020, 2020
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When CCN are injected into a turbulent cloud chamber at a constant rate, and the rate of droplet activation is balanced by the rate of droplet fallout, a steady-state droplet size distribution (DSD) can be achieved. Analytic DSDs and PDFs of droplet radius were derived for such conditions when there is uniform supersaturation. Given the chamber height, the analytic PDF is determined by the supersaturation alone. This could allow one to infer the supersaturation that produced a measured PDF.
María Cascajo-Castresana, Robert O. David, Maiara A. Iriarte-Alonso, Alexander M. Bittner, and Claudia Marcolli
Atmos. Chem. Phys., 20, 3291–3315, https://doi.org/10.5194/acp-20-3291-2020, https://doi.org/10.5194/acp-20-3291-2020, 2020
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Atmospheric ice-nucleating particles are rare but relevant for cloud glaciation. A source of particles that nucleate ice above −15 °C is biological material including some proteins. Here we show that proteins of very diverse functions and structures can nucleate ice. Among these, the iron storage protein apoferritin stands out, with activity up to −4 °C. We show that its activity does not stem from correctly assembled proteins but from misfolded protein monomers or oligomers and aggregates.
Benjamin W. Clouser, Kara D. Lamb, Laszlo C. Sarkozy, Jan Habig, Volker Ebert, Harald Saathoff, Ottmar Möhler, and Elisabeth J. Moyer
Atmos. Chem. Phys., 20, 1089–1103, https://doi.org/10.5194/acp-20-1089-2020, https://doi.org/10.5194/acp-20-1089-2020, 2020
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Previous measurements of water vapor in the upper troposphere and lower stratosphere (UT/LS) have shown unexpectedly high concentrations of water vapor in ice clouds, which may be due to an incomplete understanding of the structure of ice and the behavior of ice growth in this part of the atmosphere. Water vapor measurements during the 2013 IsoCloud campaign at the AIDA cloud chamber show no evidence of this
anomalous supersaturationin conditions similar to the real atmosphere.
Jon Nelson and Brian D. Swanson
Atmos. Chem. Phys., 19, 15285–15320, https://doi.org/10.5194/acp-19-15285-2019, https://doi.org/10.5194/acp-19-15285-2019, 2019
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Ice crystals in clouds have a wide variety. But many crystal forms are inexplicable using the common approach of modeling the growth rates normal to the crystal faces. Instead of using only this normal-growth approach, we suggest including lateral facet growth processes. Using such lateral processes, backed up by new experiments, we give explanations for some of these puzzling forms. The forms include the center droxtal in stellar crystals, scrolls, capped columns, sheath bundles, and trigonals.
Alexander D. Harrison, Katherine Lever, Alberto Sanchez-Marroquin, Mark A. Holden, Thomas F. Whale, Mark D. Tarn, James B. McQuaid, and Benjamin J. Murray
Atmos. Chem. Phys., 19, 11343–11361, https://doi.org/10.5194/acp-19-11343-2019, https://doi.org/10.5194/acp-19-11343-2019, 2019
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Mineral dusts are a source of ice-nucleating particles (INPs) in the atmosphere. Here we present a comprehensive survey of the ice-nucleating ability of naturally occurring quartz. We show the ice-nucleating variability of quartz and its sensitivity to time spent in water and air. We propose four new parameterizations for the minerals quartz, K feldspar, albite and plagioclase to predict INP concentrations in the atmosphere and show that K-feldspar is the dominant INP type in mineral dusts.
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.
Nsikanabasi Silas Umo, Robert Wagner, Romy Ullrich, Alexei Kiselev, Harald Saathoff, Peter G. Weidler, Daniel J. Cziczo, Thomas Leisner, and Ottmar Möhler
Atmos. Chem. Phys., 19, 8783–8800, https://doi.org/10.5194/acp-19-8783-2019, https://doi.org/10.5194/acp-19-8783-2019, 2019
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Annually, over 600 Tg of coal fly ash (CFA) is produced; a significant proportion of this amount is injected into the atmosphere, which could significantly contribute to heterogeneous ice formation in clouds. This study presents an improved understanding of CFA particles' behaviour in forming ice in clouds, especially when exposed to lower temperatures before being re-circulated in the upper troposphere or entrained into the lower troposphere.
Naruki Hiranuma, Kouji Adachi, David M. Bell, Franco Belosi, Hassan Beydoun, Bhaskar Bhaduri, Heinz Bingemer, Carsten Budke, Hans-Christian Clemen, Franz Conen, Kimberly M. Cory, Joachim Curtius, Paul J. DeMott, Oliver Eppers, Sarah Grawe, Susan Hartmann, Nadine Hoffmann, Kristina Höhler, Evelyn Jantsch, Alexei Kiselev, Thomas Koop, Gourihar Kulkarni, Amelie Mayer, Masataka Murakami, Benjamin J. Murray, Alessia Nicosia, Markus D. Petters, Matteo Piazza, Michael Polen, Naama Reicher, Yinon Rudich, Atsushi Saito, Gianni Santachiara, Thea Schiebel, Gregg P. Schill, Johannes Schneider, Lior Segev, Emiliano Stopelli, Ryan C. Sullivan, Kaitlyn Suski, Miklós Szakáll, Takuya Tajiri, Hans Taylor, Yutaka Tobo, Romy Ullrich, Daniel Weber, Heike Wex, Thomas F. Whale, Craig L. Whiteside, Katsuya Yamashita, Alla Zelenyuk, and Ottmar Möhler
Atmos. Chem. Phys., 19, 4823–4849, https://doi.org/10.5194/acp-19-4823-2019, https://doi.org/10.5194/acp-19-4823-2019, 2019
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A total of 20 ice nucleation measurement techniques contributed to investigate the immersion freezing behavior of cellulose particles – natural polymers. Our data showed several types of cellulose are able to nucleate ice as efficiently as some mineral dust samples and cellulose has the potential to be an important atmospheric ice-nucleating particle. Continued investigation/collaboration is necessary to obtain further insight into consistency or diversity of ice nucleation measurements.
Kaitlyn J. Suski, David M. Bell, Naruki Hiranuma, Ottmar Möhler, Dan Imre, and Alla Zelenyuk
Atmos. Chem. Phys., 18, 17497–17513, https://doi.org/10.5194/acp-18-17497-2018, https://doi.org/10.5194/acp-18-17497-2018, 2018
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This work investigates the cloud condensation nuclei and ice nucleation activity of bacteria using cloud chamber data and a single particle mass spectrometer. The size and chemical composition of the cloud residuals show that bacterial fragments mixed with agar growth media activate preferentially over intact bacteria cells as cloud condensation nuclei. Intact bacteria cells do not make it into cloud droplets; they thus cannot serve as immersion-mode ice nucleating particles.
Jiahui Zhang, Dao-Yi Gong, Rui Mao, Jing Yang, Ziyin Zhang, and Yun Qian
Atmos. Chem. Phys., 18, 16775–16791, https://doi.org/10.5194/acp-18-16775-2018, https://doi.org/10.5194/acp-18-16775-2018, 2018
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The Chinese Spring Festival (also known as the Chinese New Year or Lunar New Year) is the most important festival in China. This paper reports that during the Chinese Spring Festival, the precipitation over southern China has been significantly reduced. The precipitation reduction is due to anomalous northerly winds. We suppose that anomalous atmospheric circulation is likely related to the human activity during holidays. It is an interesting phenomenon.
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.
Jens Voigtländer, Cedric Chou, Henner Bieligk, Tina Clauss, Susan Hartmann, Paul Herenz, Dennis Niedermeier, Georg Ritter, Frank Stratmann, and Zbigniew Ulanowski
Atmos. Chem. Phys., 18, 13687–13702, https://doi.org/10.5194/acp-18-13687-2018, https://doi.org/10.5194/acp-18-13687-2018, 2018
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Surface roughness of ice crystals has recently been acknowledged to strongly influence the radiative properties of cold clouds such as cirrus, but it is unclear how this roughness arises. The study investigates the origins of ice surface roughness under a variety of atmospherically relevant conditions, using a novel method to measure roughness quantitatively. It is found that faster growth leads to stronger roughness. Roughness also increases following repeated growth–sublimation cycles.
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.
Wiebke Frey, Dawei Hu, James Dorsey, M. Rami Alfarra, Aki Pajunoja, Annele Virtanen, Paul Connolly, and Gordon McFiggans
Atmos. Chem. Phys., 18, 9393–9409, https://doi.org/10.5194/acp-18-9393-2018, https://doi.org/10.5194/acp-18-9393-2018, 2018
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The coupled system of the Manchester Aerosol Chamber and Manchester Ice Cloud Chamber was used to study the ice-forming abilities of secondary
organic aerosol particles under mixed-phase cloud conditions. Given the vast abundance of secondary organic particles in the atmosphere, they
might present an important contribution to ice-nucleating particles. However, we find that in the studied temperature range (20 to 28 °C)
the secondary organic particles do not nucleate ice particles.
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.
Pascal Lemaitre, Arnaud Querel, Marie Monier, Thibault Menard, Emmanuel Porcheron, and Andrea I. Flossmann
Atmos. Chem. Phys., 17, 4159–4176, https://doi.org/10.5194/acp-17-4159-2017, https://doi.org/10.5194/acp-17-4159-2017, 2017
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We present new measurements of the efficiency with which aerosol particles are collected by raindrops. These measurements provide the link to reconcile the scavenging coefficients obtained from theoretical approaches with those from experimental studies. We provide proof of the rear capture that is a fundamental effect on submicroscopic particles. Finally, we propose an expression to take into account this mechanism to calculate the collection efficiency for drops within the rain size range.
Lukas Kaufmann, Claudia Marcolli, Beiping Luo, and Thomas Peter
Atmos. Chem. Phys., 17, 3525–3552, https://doi.org/10.5194/acp-17-3525-2017, https://doi.org/10.5194/acp-17-3525-2017, 2017
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To improve the understanding of heterogeneous ice nucleation, we have subjected different ice nuclei to repeated freezing cycles and evaluated the freezing temperatures with different parameterizations of classical nucleation theory. It was found that two fit parameters were necessary to describe the temperature dependence of the nucleation rate.
Claudia Marcolli
Atmos. Chem. Phys., 17, 1595–1622, https://doi.org/10.5194/acp-17-1595-2017, https://doi.org/10.5194/acp-17-1595-2017, 2017
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Laboratory studies from the last century have shown that some types of particles are susceptible to pre-activation, i.e. they are able to develop macroscopic ice at warmer temperatures or lower relative humidities after they had been involved in an ice nucleation event before. This review analyses these works under the presumption that pre-activation occurs by ice preserved in pores, and it discusses atmospheric scenarios for which pre-activation might be important.
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.
Andreas Peckhaus, Alexei Kiselev, Thibault Hiron, Martin Ebert, and Thomas Leisner
Atmos. Chem. Phys., 16, 11477–11496, https://doi.org/10.5194/acp-16-11477-2016, https://doi.org/10.5194/acp-16-11477-2016, 2016
Short summary
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The precipitation in midlatitude clouds proceeds predominantly via nucleation of ice in the supercooled droplets containing foreign inclusions, like feldspar mineral dust, that have been recently identified as one of the most active ice nucleating agents in the atmosphere. We have built an apparatus to observe the freezing of feldspar immersed in up to 1500 identical droplets simultaneously. With this setup we investigated four feldspar samples and show that it can induce freezing at −5 °C.
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.
Daniel O'Sullivan, Benjamin J. Murray, James F. Ross, and Michael E. Webb
Atmos. Chem. Phys., 16, 7879–7887, https://doi.org/10.5194/acp-16-7879-2016, https://doi.org/10.5194/acp-16-7879-2016, 2016
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In the absence of particles which can trigger freezing, cloud droplets can exist in a supercooled liquid state well below the melting point. However, the sources of efficient ice-nucleating particles in the atmosphere are uncertain. Here we show that ice-nucleating proteins produced by soil fungi can bind to clay particles in soils. Hence, the subsequent dispersion of soil particles into the atmosphere acts as a route through which biological ice nucleators can influence clouds.
Kuan-Ting O and Robert Wood
Atmos. Chem. Phys., 16, 7239–7249, https://doi.org/10.5194/acp-16-7239-2016, https://doi.org/10.5194/acp-16-7239-2016, 2016
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In this work, based on the well-known formulae of classical nucleation theory (CNT), the temperature at which the mean number of critical embryos inside a droplet is unity is derived from the Boltzmann distribution function and explored as a new simplified approximation for homogeneous freezing temperature. It thus appears that the simplicity of this approximation makes it potentially useful for predicting homogeneous freezing temperatures of water droplets in the atmosphere.
Martin Schnaiter, Emma Järvinen, Paul Vochezer, Ahmed Abdelmonem, Robert Wagner, Olivier Jourdan, Guillaume Mioche, Valery N. Shcherbakov, Carl G. Schmitt, Ugo Tricoli, Zbigniew Ulanowski, and Andrew J. Heymsfield
Atmos. Chem. Phys., 16, 5091–5110, https://doi.org/10.5194/acp-16-5091-2016, https://doi.org/10.5194/acp-16-5091-2016, 2016
Leonid Nichman, Claudia Fuchs, Emma Järvinen, Karoliina Ignatius, Niko Florian Höppel, Antonio Dias, Martin Heinritzi, Mario Simon, Jasmin Tröstl, Andrea Christine Wagner, Robert Wagner, Christina Williamson, Chao Yan, Paul James Connolly, James Robert Dorsey, Jonathan Duplissy, Sebastian Ehrhart, Carla Frege, Hamish Gordon, Christopher Robert Hoyle, Thomas Bjerring Kristensen, Gerhard Steiner, Neil McPherson Donahue, Richard Flagan, Martin William Gallagher, Jasper Kirkby, Ottmar Möhler, Harald Saathoff, Martin Schnaiter, Frank Stratmann, and António Tomé
Atmos. Chem. Phys., 16, 3651–3664, https://doi.org/10.5194/acp-16-3651-2016, https://doi.org/10.5194/acp-16-3651-2016, 2016
Short summary
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Processes in the atmosphere are often governed by the physical and chemical properties of small cloud particles. Ice, water, and mixed clouds, as well as viscous aerosols, were formed under controlled conditions at the CLOUD-CERN facility. The experimental results show a link between cloud particle properties and their unique optical fingerprints. The classification map presented here allows easier discrimination between various particles such as viscous organic aerosol, salt, ice, and liquid.
Robert Wagner, Alexei Kiselev, Ottmar Möhler, Harald Saathoff, and Isabelle Steinke
Atmos. Chem. Phys., 16, 2025–2042, https://doi.org/10.5194/acp-16-2025-2016, https://doi.org/10.5194/acp-16-2025-2016, 2016
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We have investigated the enhancement of the ice nucleation ability of well-known and abundant ice nucleating particles like dust grains due to pre-activation. Temporary exposure to a low temperature (228 K) provokes that pores and surface cracks of the particles are filled with ice, which makes them better nuclei for the growth of macroscopic ice crystals at high temperatures (245–260 K).
M. L. López and E. E. Ávila
Atmos. Chem. Phys., 16, 927–932, https://doi.org/10.5194/acp-16-927-2016, https://doi.org/10.5194/acp-16-927-2016, 2016
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This work deals with the origin and nature of atmospheric ice-nucleating particles (INPs). An accurate determination of the atmospheric INP concentration is relevant since INPs induce freezing in clouds, thus initiating an efficient mechanism for cloud particles to reach a precipitating size.
The effect of relative humidity on the INP concentration at ground level was analyzed and discussed.
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.
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Short summary
A stochastic immersion freezing model is introduced capable of reproducing laboratory data for a variety of experimental methods using a time and surface area dependent ice nucleation process. The assumption that droplets contain identical surface area is evaluated. A quantitative uncertainty analysis of the laboratory observed freezing process is presented. Our results imply that ice nuclei surface area assumptions are crucial for interpretation of experimental immersion freezing results.
A stochastic immersion freezing model is introduced capable of reproducing laboratory data for a...
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