Articles | Volume 25, issue 23
https://doi.org/10.5194/acp-25-18249-2025
© Author(s) 2025. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Special issue:
https://doi.org/10.5194/acp-25-18249-2025
© Author(s) 2025. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Volume uptake of carbonyls during diffusional ice crystal growth
Institute for Atmospheric Physics, Johannes Gutenberg University, Mainz, Germany
Miklós Szakáll
Institute for Atmospheric Physics, Johannes Gutenberg University, Mainz, Germany
Alexander Theis
Particle Chemistry Department, Max Planck Institute for Chemistry, Mainz, Germany
Subir K. Mitra
Particle Chemistry Department, Max Planck Institute for Chemistry, Mainz, Germany
Christine Borchers
Department of Chemistry, Johannes Gutenberg University, Mainz, Germany
Thorsten Hoffmann
Department of Chemistry, Johannes Gutenberg University, Mainz, Germany
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Martanda Gautam, Alexander Theis, Jackson Seymore, Moritz Hey, Stephan Borrmann, Karoline Diehl, Subir K. Mitra, and Miklós Szakáll
Atmos. Chem. Phys., 25, 11813–11828, https://doi.org/10.5194/acp-25-11813-2025, https://doi.org/10.5194/acp-25-11813-2025, 2025
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We investigated the retention of chemical species and their binary mixtures during freezing of raindrops via acoustic levitation. Our results reveal high retention, with nearly all substances being fully retained during freezing. This could be attributed to a faster freezing time compared to a slower mass expulsion time, along with ice shell formation during freezing. This result helps improve our understanding of the interaction between ice microphysical processes and chemistry in deep convective clouds.
Jackson Seymore, Martanda Gautam, Miklós Szakáll, Alexander Theis, Thorsten Hoffmann, Jialiang Ma, Lingli Zhou, and Alexander L. Vogel
Atmos. Chem. Phys., 25, 11829–11845, https://doi.org/10.5194/acp-25-11829-2025, https://doi.org/10.5194/acp-25-11829-2025, 2025
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We investigated the chemical retention of water-soluble organic compounds in Beijing aerosols using an acoustic levitator and drop-freezing experiments. Samples from PM2.5 filter extracts were frozen at -15 °C in an acoustic levitator without artificial nucleators and analyzed using ultra-high resolution mass spectrometry. Our findings reveal a non-normal distribution of retention coefficients that differs from current literature on cloud droplets.
Christine Borchers, Jackson Seymore, Martanda Gautam, Konstantin Dörholt, Yannik Müller, Andreas Arndt, Laura Gömmer, Florian Ungeheuer, Miklós Szakáll, Stephan Borrmann, Alexander Theis, Alexander L. Vogel, and Thorsten Hoffmann
Atmos. Chem. Phys., 24, 13961–13974, https://doi.org/10.5194/acp-24-13961-2024, https://doi.org/10.5194/acp-24-13961-2024, 2024
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Riming, a crucial process in cloud dynamics, influences the vertical distribution of compounds in the atmosphere. Experiments in Mainz's wind tunnel investigated retention coefficients of organic compounds under varying conditions. Findings suggest a correlation between the Henry's law constant and retention, applicable even to complex organic molecules.
Christine Borchers, Lasse Moormann, Bastien Geil, Niklas Karbach, David Wasserzier, and Thorsten Hoffmann
Atmos. Meas. Tech., 18, 7231–7242, https://doi.org/10.5194/amt-18-7231-2025, https://doi.org/10.5194/amt-18-7231-2025, 2025
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A three-dimensionally printed filter holder is connected to a lightweight, high-performance pump. This sampling system allows for easy and cost-effective measurements of organic aerosols at different heights and locations. By elucidating the chemical composition of organic aerosol, sources and processing of the compounds can be identified. Measurements at different altitudes and times of the day provide insight into the chemical aging and daytime trends of the aerosol particles.
Anna Breuninger, Philipp Joppe, Jonas Wilsch, Cornelis Schwenk, Heiko Bozem, Nicolas Emig, Laurin Merkel, Rainer Rossberg, Timo Keber, Arthur Kutschka, Philipp Waleska, Stefan Hofmann, Sarah Richter, Florian Ungeheuer, Konstantin Dörholt, Thorsten Hoffmann, Annette Miltenberger, Johannes Schneider, Peter Hoor, and Alexander L. Vogel
Atmos. Chem. Phys., 25, 16533–16551, https://doi.org/10.5194/acp-25-16533-2025, https://doi.org/10.5194/acp-25-16533-2025, 2025
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This study investigates molecular organic aerosol composition in the upper troposphere and lower stratosphere from an airborne campaign over Central Europe in summer 2024. Via ultra-high-performance liquid chromatography and high-resolution mass spectrometry of tropospheric and stratospheric filter samples, we identified various organic compounds. Our findings underscore the significant cross-tropopause transport of biogenic secondary organic aerosol and anthropogenic pollutants.
Martanda Gautam, Alexander Theis, Jackson Seymore, Moritz Hey, Stephan Borrmann, Karoline Diehl, Subir K. Mitra, and Miklós Szakáll
Atmos. Chem. Phys., 25, 11813–11828, https://doi.org/10.5194/acp-25-11813-2025, https://doi.org/10.5194/acp-25-11813-2025, 2025
Short summary
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We investigated the retention of chemical species and their binary mixtures during freezing of raindrops via acoustic levitation. Our results reveal high retention, with nearly all substances being fully retained during freezing. This could be attributed to a faster freezing time compared to a slower mass expulsion time, along with ice shell formation during freezing. This result helps improve our understanding of the interaction between ice microphysical processes and chemistry in deep convective clouds.
Jackson Seymore, Martanda Gautam, Miklós Szakáll, Alexander Theis, Thorsten Hoffmann, Jialiang Ma, Lingli Zhou, and Alexander L. Vogel
Atmos. Chem. Phys., 25, 11829–11845, https://doi.org/10.5194/acp-25-11829-2025, https://doi.org/10.5194/acp-25-11829-2025, 2025
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We investigated the chemical retention of water-soluble organic compounds in Beijing aerosols using an acoustic levitator and drop-freezing experiments. Samples from PM2.5 filter extracts were frozen at -15 °C in an acoustic levitator without artificial nucleators and analyzed using ultra-high resolution mass spectrometry. Our findings reveal a non-normal distribution of retention coefficients that differs from current literature on cloud droplets.
Maja Rüth, Nicole Bobrowski, Ellen Bräutigam, Alexander Nies, Jonas Kuhn, Thorsten Hoffmann, Niklas Karbach, Bastien Geil, Ralph Kleinschek, Stefan Schmitt, and Ulrich Platt
EGUsphere, https://doi.org/10.5194/egusphere-2025-3976, https://doi.org/10.5194/egusphere-2025-3976, 2025
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UV absorption and electrochemical O3 sensor measurement techniques suffer from interferences, especially from SO2, which is a main constituent of volcanic plumes. Only chemiluminescence (CL) O3 monitors have no known interference with SO2. However, modern CL O3 monitors are impractical because they are heavy and bulky. We developed and applied a lightweight version of a CL O3 instrument (l.5 kg, shoebox size) and present the result of those drone based CL O3 measurements.
Sudha Yadav, Lilly Metten, Pierre Grzegorczyk, Alexander Theis, Subir K. Mitra, and Miklós Szakáll
Atmos. Chem. Phys., 25, 8671–8682, https://doi.org/10.5194/acp-25-8671-2025, https://doi.org/10.5194/acp-25-8671-2025, 2025
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Laboratory studies on the fragmentation of ice particles by collision are presented. Graupel particles were created by riming at –7 and –15 °C, also simulating rotation and tumbling. Frozen ice drops were generated by freezing water in 3D-printed spherical molds. The number of fragments generated by collision was between 1 and 20 and was strongly dependent on the density of the graupel. We also showed that the number of fragments approaches zero when the particle suffers more than three collisions in a row.
Jade Margerum, Julia Homann, Stuart Umbo, Gernot Nehrke, Thorsten Hoffmann, Anton Vaks, Aleksandr Kononov, Alexander Osintsev, Alena Giesche, Andrew Mason, Franziska A. Lechleitner, Gideon M. Henderson, Ola Kwiecien, and Sebastian F. M. Breitenbach
Clim. Past, 21, 661–677, https://doi.org/10.5194/cp-21-661-2025, https://doi.org/10.5194/cp-21-661-2025, 2025
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We analyse a southern Siberian stalagmite to reconstruct soil respiration, wildfire, and vegetation trends during the Last Interglacial (LIG) (124.1–118.8 ka) and the Holocene (10–0 ka). Wildfires were more prevalent during the LIG than the Holocene and were supported by fire-prone species, low soil respiration, and a greater difference between summer and winter temperature. We show that vegetation type and summer/winter temperature contrast are strong drivers of Siberian wildfires.
Denis Leppla, Stefanie Hildmann, Nora Zannoni, Leslie Kremper, Bruna Hollanda, Jonathan Williams, Christopher Pöhlker, Stefan Wolff, Marta Sà, Maria Cristina Solci, Ulrich Pöschl, and Thorsten Hoffmann
EGUsphere, https://doi.org/10.5194/egusphere-2025-141, https://doi.org/10.5194/egusphere-2025-141, 2025
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The chemical composition of organic particles in the Amazon rainforest was investigated to understand how biogenic and human emissions influence the atmosphere in this unique ecosystem. Seasonal patterns were found where wet seasons were dominated by biogenic compounds from natural sources while dry seasons showed increased fire-related pollutants. These findings reveal how emissions, fires and long-range transport affect atmospheric chemistry, with implications for climate models.
Johanna Schäfer, Anja Beschnitt, François Burgay, Thomas Singer, Margit Schwikowski, and Thorsten Hoffmann
Atmos. Meas. Tech., 18, 421–430, https://doi.org/10.5194/amt-18-421-2025, https://doi.org/10.5194/amt-18-421-2025, 2025
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Glaciers preserve organic compounds from atmospheric aerosols, which can serve as markers for emission sources. Most studies overlook the enantiomers of chiral compounds. We developed a two-dimensional liquid chromatography method to determine the chiral ratios of the monoterpene oxidation products cis-pinic acid and cis-pinonic acid in ice-core samples. Applied to samples from the Belukha Glacier (1870–1970 CE), the method revealed fluctuating chiral ratios for the analytes.
Christine Borchers, Jackson Seymore, Martanda Gautam, Konstantin Dörholt, Yannik Müller, Andreas Arndt, Laura Gömmer, Florian Ungeheuer, Miklós Szakáll, Stephan Borrmann, Alexander Theis, Alexander L. Vogel, and Thorsten Hoffmann
Atmos. Chem. Phys., 24, 13961–13974, https://doi.org/10.5194/acp-24-13961-2024, https://doi.org/10.5194/acp-24-13961-2024, 2024
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Riming, a crucial process in cloud dynamics, influences the vertical distribution of compounds in the atmosphere. Experiments in Mainz's wind tunnel investigated retention coefficients of organic compounds under varying conditions. Findings suggest a correlation between the Henry's law constant and retention, applicable even to complex organic molecules.
Niklas Karbach, Lisa Höhler, Peter Hoor, Heiko Bozem, Nicole Bobrowski, and Thorsten Hoffmann
Atmos. Meas. Tech., 17, 4081–4086, https://doi.org/10.5194/amt-17-4081-2024, https://doi.org/10.5194/amt-17-4081-2024, 2024
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The system presented here can accurately generate and reproduce a stable flow of gas mixtures of known concentrations over several days using ambient air as a dilution medium. In combination with the small size and low weight of the system, this enables the calibration of hydrogen sensors in the field, reducing the influence of matrix effects on the accuracy of the sensor. The system is inexpensive to assemble and easy to maintain, which is the key to reliable measurement results.
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.
Julia Homann, Niklas Karbach, Stacy A. Carolin, Daniel H. James, David Hodell, Sebastian F. M. Breitenbach, Ola Kwiecien, Mark Brenner, Carlos Peraza Lope, and Thorsten Hoffmann
Biogeosciences, 20, 3249–3260, https://doi.org/10.5194/bg-20-3249-2023, https://doi.org/10.5194/bg-20-3249-2023, 2023
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Cave stalagmites contain substances that can be used to reconstruct past changes in local and regional environmental conditions. We used two classes of biomarkers (polycyclic aromatic hydrocarbons and monosaccharide anhydrides) to detect the presence of fire and to also explore changes in fire regime (e.g. fire frequency, intensity, and fuel source). We tested our new method on a stalagmite from Mayapan, a large Maya city on the Yucatán Peninsula.
Denis Leppla, Nora Zannoni, Leslie Kremper, Jonathan Williams, Christopher Pöhlker, Marta Sá, Maria Christina Solci, and Thorsten Hoffmann
Atmos. Chem. Phys., 23, 809–820, https://doi.org/10.5194/acp-23-809-2023, https://doi.org/10.5194/acp-23-809-2023, 2023
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Chiral chemodiversity plays a critical role in biochemical processes such as insect and plant communication. Here we report on the measurement of chiral-specified secondary organic aerosol in the Amazon rainforest. The results show that the chiral ratio is mainly determined by large-scale emission processes. Characteristic emissions of chiral aerosol precursors from different forest ecosystems can thus provide large-scale information on different biogenic sources via chiral particle analysis.
Yunfan Liu, Hang Su, Siwen Wang, Chao Wei, Wei Tao, Mira L. Pöhlker, Christopher Pöhlker, Bruna A. Holanda, Ovid O. Krüger, Thorsten Hoffmann, Manfred Wendisch, Paulo Artaxo, Ulrich Pöschl, Meinrat O. Andreae, and Yafang Cheng
Atmos. Chem. Phys., 23, 251–272, https://doi.org/10.5194/acp-23-251-2023, https://doi.org/10.5194/acp-23-251-2023, 2023
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The origins of the abundant cloud condensation nuclei (CCN) in the upper troposphere (UT) of the Amazon remain unclear. With model developments of new secondary organic aerosol schemes and constrained by observation, we show that strong aerosol nucleation and condensation in the UT is triggered by biogenic organics, and organic condensation is key for UT CCN production. This UT CCN-producing mechanism may prevail over broader vegetation canopies and deserves emphasis in aerosol–climate feedback.
Jing Duan, Ru-Jin Huang, Yifang Gu, Chunshui Lin, Haobin Zhong, Wei Xu, Quan Liu, Yan You, Jurgita Ovadnevaite, Darius Ceburnis, Thorsten Hoffmann, and Colin O'Dowd
Atmos. Chem. Phys., 22, 10139–10153, https://doi.org/10.5194/acp-22-10139-2022, https://doi.org/10.5194/acp-22-10139-2022, 2022
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Biomass-burning-influenced oxygenated organic aerosol (OOA-BB), formed from the photochemical oxidation and aging of biomass burning OA (BBOA), was resolved in urban Xi’an. The aqueous-phase processed oxygenated OA (aq-OOA) concentration was more dependent on secondary inorganic aerosol (SIA) content and aerosol liquid water content (ALWC). The increased aq-OOA contribution during SIA-enhanced periods likely reflects OA evolution due to the addition of alcohol or peroxide groups
Alexandra Gutmann, Nicole Bobrowski, Marcello Liotta, and Thorsten Hoffmann
Atmos. Meas. Tech., 14, 6395–6406, https://doi.org/10.5194/amt-14-6395-2021, https://doi.org/10.5194/amt-14-6395-2021, 2021
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Motivated by a special interest in bromine chemistry in volcanic plumes, the study presented here describes a new method for the quantitative collection of gaseous hydrogen bromide in gas diffusion denuders. The hydrogen bromide reacted during sampling with appropriate epoxides applied to the denuder walls. The denuder sampling assembly was successfully deployed in the volcanic plume of Masaya volcano, Nicaragua.
Haijie Tong, Fobang Liu, Alexander Filippi, Jake Wilson, Andrea M. Arangio, Yun Zhang, Siyao Yue, Steven Lelieveld, Fangxia Shen, Helmi-Marja K. Keskinen, Jing Li, Haoxuan Chen, Ting Zhang, Thorsten Hoffmann, Pingqing Fu, William H. Brune, Tuukka Petäjä, Markku Kulmala, Maosheng Yao, Thomas Berkemeier, Manabu Shiraiwa, and Ulrich Pöschl
Atmos. Chem. Phys., 21, 10439–10455, https://doi.org/10.5194/acp-21-10439-2021, https://doi.org/10.5194/acp-21-10439-2021, 2021
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We measured radical yields of aqueous PM2.5 extracts and found lower yields at higher concentrations of PM2.5. Abundances of water-soluble transition metals and aromatics in PM2.5 were positively correlated with the relative fraction of •OH but negatively correlated with the relative fraction of C-centered radicals among detected radicals. Composition-dependent reactive species yields may explain differences in the reactivity and health effects of PM2.5 in clean versus polluted air.
Kai Wang, Ru-Jin Huang, Martin Brüggemann, Yun Zhang, Lu Yang, Haiyan Ni, Jie Guo, Meng Wang, Jiajun Han, Merete Bilde, Marianne Glasius, and Thorsten Hoffmann
Atmos. Chem. Phys., 21, 9089–9104, https://doi.org/10.5194/acp-21-9089-2021, https://doi.org/10.5194/acp-21-9089-2021, 2021
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Here we present the detailed molecular composition of the organic aerosol collected in three eastern Chinese cities from north to south, Changchun, Shanghai and Guangzhou, by applying LC–Orbitrap analysis. Accordingly, the aromaticity degree of chemical compounds decreases from north to south, while the oxidation degree increases from north to south, which can be explained by the different anthropogenic emissions and photochemical oxidation processes.
Bo Galle, Santiago Arellano, Nicole Bobrowski, Vladimir Conde, Tobias P. Fischer, Gustav Gerdes, Alexandra Gutmann, Thorsten Hoffmann, Ima Itikarai, Tomas Krejci, Emma J. Liu, Kila Mulina, Scott Nowicki, Tom Richardson, Julian Rüdiger, Kieran Wood, and Jiazhi Xu
Atmos. Meas. Tech., 14, 4255–4277, https://doi.org/10.5194/amt-14-4255-2021, https://doi.org/10.5194/amt-14-4255-2021, 2021
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Measurements of volcanic gases are important for geophysical research, risk assessment and environmental impact studies. Some gases, like SO2 and BrO, may be studied from the ground at a safe distance using remote sensing techniques. Many other gases require in situ access to the gas plume. Here, a drone may be an attractive alternative. This paper describes a drone specially adapted for volcanic gas studies and demonstrates its use in a field campaign at Manam volcano in Papua New Guinea.
Inken Heidke, Adam Hartland, Denis Scholz, Andrew Pearson, John Hellstrom, Sebastian F. M. Breitenbach, and Thorsten Hoffmann
Biogeosciences, 18, 2289–2300, https://doi.org/10.5194/bg-18-2289-2021, https://doi.org/10.5194/bg-18-2289-2021, 2021
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We analyzed lignin oxidation products (LOPs) in leaf litter and different soil horizons as well as dripwater and flowstone samples from four different cave sites from different vegetation zones in New Zealand using liquid chromatography coupled to mass spectrometry. We test whether the original source-dependent LOP signal of the overlying vegetation is preserved and can be recovered from flowstone samples and investigate how the signal is altered by the transport from the soil to the cave.
Wei Yuan, Ru-Jin Huang, Lu Yang, Ting Wang, Jing Duan, Jie Guo, Haiyan Ni, Yang Chen, Qi Chen, Yongjie Li, Ulrike Dusek, Colin O'Dowd, and Thorsten Hoffmann
Atmos. Chem. Phys., 21, 3685–3697, https://doi.org/10.5194/acp-21-3685-2021, https://doi.org/10.5194/acp-21-3685-2021, 2021
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We characterized the seasonal variations in nitrated aromatic compounds (NACs) in composition, sources, and their light absorption contribution to brown carbon (BrC) aerosol in Xi'an, Northwest China. Our results show that secondary formation and vehicular emission were dominant sources in summer (~80 %), and biomass burning and coal combustion were major sources in winter (~75 %), and they indicate that the composition and sources of NACs have a profound impact on the light absorption of BrC
Julian Rüdiger, Alexandra Gutmann, Nicole Bobrowski, Marcello Liotta, J. Maarten de Moor, Rolf Sander, Florian Dinger, Jan-Lukas Tirpitz, Martha Ibarra, Armando Saballos, María Martínez, Elvis Mendoza, Arnoldo Ferrufino, John Stix, Juan Valdés, Jonathan M. Castro, and Thorsten Hoffmann
Atmos. Chem. Phys., 21, 3371–3393, https://doi.org/10.5194/acp-21-3371-2021, https://doi.org/10.5194/acp-21-3371-2021, 2021
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We present an innovative approach to study halogen chemistry in the plume of Masaya volcano in Nicaragua. An unique data set was collected using multiple techniques, including drones. These data enabled us to determine the fraction of activation of the respective halogens at various plume ages, where in-mixing of ambient air causes chemical reactions. An atmospheric chemistry box model was employed to further examine the field results and help our understanding of volcanic plume chemistry.
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.
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Short summary
Laboratory studies examined carbonyl deposition into ice crystals using a flowtube setup. Ice crystals were grown under conditions that mimic cirrus clouds in the presence of carbonyl vapors. Ice and gas samples were collected and analyzed to calculate ice uptake coefficients for 14 carbonyls at different temperatures. This revealed an inverse relationship between uptake and temperature. Vapor pressure and molar mass were found to be the most significant factors in uptake.
Laboratory studies examined carbonyl deposition into ice crystals using a flowtube setup. Ice...
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