Articles | Volume 18, issue 13
https://doi.org/10.5194/acp-18-9393-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-18-9393-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
05 Jul 2018
Research article |
| 05 Jul 2018
| 05 Jul 2018
The efficiency of secondary organic aerosol particles acting as ice-nucleating particles under mixed-phase cloud conditions
Centre for Atmospheric Science, School of Earth and Environmental Sciences, The University of Manchester, Manchester, UK
now at: Leibniz Institute for Tropospheric Research (TROPOS), Leipzig, Germany
Dawei Hu
Centre for Atmospheric Science, School of Earth and Environmental Sciences, The University of Manchester, Manchester, UK
James Dorsey
Centre for Atmospheric Science, School of Earth and Environmental Sciences, The University of Manchester, Manchester, UK
M. Rami Alfarra
Centre for Atmospheric Science, School of Earth and Environmental Sciences, The University of Manchester, Manchester, UK
National Centre for Atmospheric Science (NCAS), The University of Manchester, Manchester, UK
Aki Pajunoja
Department of Applied Physics, University of Eastern Finland, Kuopio, Finland
Annele Virtanen
Department of Applied Physics, University of Eastern Finland, Kuopio, Finland
Paul Connolly
Centre for Atmospheric Science, School of Earth and Environmental Sciences, The University of Manchester, Manchester, UK
Gordon McFiggans
Centre for Atmospheric Science, School of Earth and Environmental Sciences, The University of Manchester, Manchester, UK
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This paper shows the specific impact of black carbon (BC) on the aerosol–planetary boundary layer (PBL) feedback and its influence on a Beijing haze episode. Overall, this paper shows that strong temperature inversions prevent BC heating within the PBL from significantly increasing PBL height, while BC above the PBL suppresses PBL development significantly through the day. From this we suggest a method by which both locally and regionally emitted BC may impact urban pollution episodes.
Kimmo Korhonen, Thomas Bjerring Kristensen, John Falk, Vilhelm B. Malmborg, Axel Eriksson, Louise Gren, Maja Novakovic, Sam Shamun, Panu Karjalainen, Lassi Markkula, Joakim Pagels, Birgitta Svenningsson, Martin Tunér, Mika Komppula, Ari Laaksonen, and Annele Virtanen
Atmos. Chem. Phys., 22, 1615–1631, https://doi.org/10.5194/acp-22-1615-2022, https://doi.org/10.5194/acp-22-1615-2022, 2022
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We investigated the ice-nucleating abilities of particulate emissions from a modern diesel engine using the portable ice-nuclei counter SPIN, a continuous-flow diffusion chamber instrument. Three different fuels were studied without blending, including fossil diesel and two renewable fuels, testing different emission aftertreatment systems and photochemical aging. We found that the diesel emissions were inefficient ice nuclei, and aging had no or little effect on their ice-nucleating abilities.
Yunqi Shao, Yu Wang, Mao Du, Aristeidis Voliotis, M. Rami Alfarra, Simon P. O'Meara, S. Fiona Turner, and Gordon McFiggans
Atmos. Meas. Tech., 15, 539–559, https://doi.org/10.5194/amt-15-539-2022, https://doi.org/10.5194/amt-15-539-2022, 2022
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A comprehensive description and characterisation of the Manchester Aerosol Chamber (MAC) was conducted. The MAC has good temperature and relative humidity homogeneity, fast mixing times, and comparable losses of gases and particles with other chambers. The MAC's bespoke control system allows improved duty cycles and repeatable experiments. Moreover, the effect of contamination on performance was also investigated. It is highly recommended to regularly track the chamber's performance.
Noora Hyttinen, Iida Pullinen, Aki Nissinen, Siegfried Schobesberger, Annele Virtanen, and Taina Yli-Juuti
Atmos. Chem. Phys., 22, 1195–1208, https://doi.org/10.5194/acp-22-1195-2022, https://doi.org/10.5194/acp-22-1195-2022, 2022
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Accurate saturation vapor pressure estimates of atmospherically relevant organic compounds are critical for modeling secondary organic aerosol (SOA) formation. We investigated vapor pressures of highly oxygenated SOA constituents using state-of-the-art computational and experimental methods. We found a good agreement between low and extremely low vapor pressures estimated using the two methods, and the smallest molecules detected in our experiment were likely products of thermal decomposition.
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.
Zijun Li, Angela Buchholz, Arttu Ylisirniö, Luis Barreira, Liqing Hao, Siegfried Schobesberger, Taina Yli-Juuti, and Annele Virtanen
Atmos. Chem. Phys., 21, 18283–18302, https://doi.org/10.5194/acp-21-18283-2021, https://doi.org/10.5194/acp-21-18283-2021, 2021
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We compared the evolution of two types of secondary organic aerosol (SOA) particles during isothermal evaporation. The sesquiterpene SOA particles demonstrated higher resilience to evaporation than α-pinene SOA particles generated under comparable conditions. In-depth analysis showed that under high-relative-humidity conditions, particulate water drove the evolution of particulate constituents by reducing the particle viscosity and initiating chemical aqueous-phase processes.
Dawei Hu, M. Rami Alfarra, Kate Szpek, Justin M. Langridge, Michael I. Cotterell, Claire Belcher, Ian Rule, Zixia Liu, Chenjie Yu, Yunqi Shao, Aristeidis Voliotis, Mao Du, Brett Smith, Greg Smallwood, Prem Lobo, Dantong Liu, Jim M. Haywood, Hugh Coe, and James D. Allan
Atmos. Chem. Phys., 21, 16161–16182, https://doi.org/10.5194/acp-21-16161-2021, https://doi.org/10.5194/acp-21-16161-2021, 2021
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Here, we developed new techniques for investigating these properties in the laboratory and applied these to BC and BrC from different sources, including diesel exhaust, inverted propane flame and wood combustion. These have allowed us to quantify the changes in shape and chemical composition of different soots according to source and variables such as the moisture content of wood.
Aristeidis Voliotis, Yu Wang, Yunqi Shao, Mao Du, Thomas J. Bannan, Carl J. Percival, Spyros N. Pandis, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 21, 14251–14273, https://doi.org/10.5194/acp-21-14251-2021, https://doi.org/10.5194/acp-21-14251-2021, 2021
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Secondary organic aerosol (SOA) formation from mixtures of volatile precursors can be affected by the molecular interactions of the products. Composition and volatility measurements of SOA formed from mixtures of anthropogenic and biogenic precursors reveal processes that can increase or decrease the SOA volatility. The unique products of the mixture were more oxygenated and less volatile than those from either precursor. Analytical context is provided to explore the SOA volatility in mixtures.
Ernesto Reyes-Villegas, Upasana Panda, Eoghan Darbyshire, James M. Cash, Rutambhara Joshi, Ben Langford, Chiara F. Di Marco, Neil J. Mullinger, Mohammed S. Alam, Leigh R. Crilley, Daniel J. Rooney, W. Joe F. Acton, Will Drysdale, Eiko Nemitz, Michael Flynn, Aristeidis Voliotis, Gordon McFiggans, Hugh Coe, James Lee, C. Nicholas Hewitt, Mathew R. Heal, Sachin S. Gunthe, Tuhin K. Mandal, Bhola R. Gurjar, Shivani, Ranu Gadi, Siddhartha Singh, Vijay Soni, and James D. Allan
Atmos. Chem. Phys., 21, 11655–11667, https://doi.org/10.5194/acp-21-11655-2021, https://doi.org/10.5194/acp-21-11655-2021, 2021
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This paper shows the first multisite online measurements of PM1 in Delhi, India, with measurements over different seasons in Old Delhi and New Delhi in 2018. Organic aerosol (OA) source apportionment was performed using positive matrix factorisation (PMF). Traffic was the main primary aerosol source for both OAs and black carbon, seen with PMF and Aethalometer model analysis, indicating that control of primary traffic exhaust emissions would make a significant reduction to Delhi air pollution.
Yu Wang, Aristeidis Voliotis, Yunqi Shao, Taomou Zong, Xiangxinyue Meng, Mao Du, Dawei Hu, Ying Chen, Zhijun Wu, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 21, 11303–11316, https://doi.org/10.5194/acp-21-11303-2021, https://doi.org/10.5194/acp-21-11303-2021, 2021
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Aerosol phase behaviour plays a profound role in atmospheric physicochemical processes. We designed dedicated chamber experiments to study the phase state of secondary organic aerosol from biogenic and anthropogenic mixed precursors. Our results highlight the key role of the organic–inorganic ratio and relative humidity in phase state, but the sources and organic composition are less important. The result provides solid laboratory evidence for understanding aerosol phase in a complex atmosphere.
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.
Michael Priestley, Thomas J. Bannan, Michael Le Breton, Stephen D. Worrall, Sungah Kang, Iida Pullinen, Sebastian Schmitt, Ralf Tillmann, Einhard Kleist, Defeng Zhao, Jürgen Wildt, Olga Garmash, Archit Mehra, Asan Bacak, Dudley E. Shallcross, Astrid Kiendler-Scharr, Åsa M. Hallquist, Mikael Ehn, Hugh Coe, Carl J. Percival, Mattias Hallquist, Thomas F. Mentel, and Gordon McFiggans
Atmos. Chem. Phys., 21, 3473–3490, https://doi.org/10.5194/acp-21-3473-2021, https://doi.org/10.5194/acp-21-3473-2021, 2021
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A significant fraction of emissions from human activity consists of aromatic hydrocarbons, e.g. benzene, which oxidise to form new compounds important for particle growth. Characterisation of benzene oxidation products highlights the range of species produced as well as their chemical properties and contextualises them within relevant frameworks, e.g. MCM. Cluster analysis of the oxidation product time series distinguishes behaviours of CHON compounds that could aid in identifying functionality.
Antti Ruuskanen, Sami Romakkaniemi, Harri Kokkola, Antti Arola, Santtu Mikkonen, Harri Portin, Annele Virtanen, Kari E. J. Lehtinen, Mika Komppula, and Ari Leskinen
Atmos. Chem. Phys., 21, 1683–1695, https://doi.org/10.5194/acp-21-1683-2021, https://doi.org/10.5194/acp-21-1683-2021, 2021
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The study focuses mainly on cloud-scavenging efficiency of absorbing particulate matter (mainly black carbon) but additionally covers cloud-scavenging efficiency of scattering particles and statistics of cloud condensation nuclei. The main findings give insight into how black carbon is distributed in different particle sizes and the sensitivity to cloud scavenged. The main findings are useful for large-scale modelling for evaluating cloud scavenging.
Simon Patrick O'Meara, Shuxuan Xu, David Topping, M. Rami Alfarra, Gerard Capes, Douglas Lowe, Yunqi Shao, and Gordon McFiggans
Geosci. Model Dev., 14, 675–702, https://doi.org/10.5194/gmd-14-675-2021, https://doi.org/10.5194/gmd-14-675-2021, 2021
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User-friendly and open-source software for simulating aerosol chambers is a valuable tool for research scientists in designing and analysing their experiments. This paper describes a new version of such software and will therefore provide a useful reference for those applying it. Central to the paper is an assessment of the software's accuracy through comparison against previously published simulations.
Arttu Ylisirniö, Luis M. F. Barreira, Iida Pullinen, Angela Buchholz, John Jayne, Jordan E. Krechmer, Douglas R. Worsnop, Annele Virtanen, and Siegfried Schobesberger
Atmos. Meas. Tech., 14, 355–367, https://doi.org/10.5194/amt-14-355-2021, https://doi.org/10.5194/amt-14-355-2021, 2021
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FIGAERO-ToF-CIMS enables online volatility measurements of chemical compounds in ambient aerosols. Previously published volatility calibration results however differ from each other significantly. In this study we investigate the reason for this discrepancy. We found a major source of error in the widely used syringe deposition method and propose a new method for volatility calibration by using atomized calibration compounds.
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.
Liqing Hao, Eetu Kari, Ari Leskinen, Douglas R. Worsnop, and Annele Virtanen
Atmos. Chem. Phys., 20, 14393–14405, https://doi.org/10.5194/acp-20-14393-2020, https://doi.org/10.5194/acp-20-14393-2020, 2020
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Our work presents the observational results of secondary organic aerosol (SOA) formation in the presence of ammonia. The particle-phase ammonium was continuously produced even after SOA formation had ceased. The gas-phase organic acids were observed to contribute to the formed particle-phase ammonium salts. This study suggests that the presence of ammonia may change the mass and chemical composition of large-size SOA particles and can potentially alter the aerosol impact on climate change.
Jessica Slater, Juha Tonttila, Gordon McFiggans, Paul Connolly, Sami Romakkaniemi, Thomas Kühn, and Hugh Coe
Atmos. Chem. Phys., 20, 11893–11906, https://doi.org/10.5194/acp-20-11893-2020, https://doi.org/10.5194/acp-20-11893-2020, 2020
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The feedback effect between aerosol particles, radiation and meteorology reduces turbulent motion and results in increased surface aerosol concentrations during Beijing haze. Observational analysis and regional modelling studies have examined the feedback effect but these studies are limited. In this work, we set up a high-resolution model for the Beijing environment to examine the sensitivity of the aerosol feedback effect to initial meteorological conditions and aerosol loading.
Martin Heinritzi, Lubna Dada, Mario Simon, Dominik Stolzenburg, Andrea C. Wagner, Lukas Fischer, Lauri R. Ahonen, Stavros Amanatidis, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Bernhard Baumgartner, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, Antonio Dias, Josef Dommen, Jonathan Duplissy, Henning Finkenzeller, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Manuel Granzin, Imad El Haddad, Xucheng He, Johanna Helm, Victoria Hofbauer, Christopher R. Hoyle, Juha Kangasluoma, Timo Keber, Changhyuk Kim, Andreas Kürten, Houssni Lamkaddam, Tiia M. Laurila, Janne Lampilahti, Chuan Ping Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Vladimir Makhmutov, Hanna Elina Manninen, Ruby Marten, Serge Mathot, Roy Lee Mauldin, Bernhard Mentler, Ugo Molteni, Tatjana Müller, Wei Nie, Tuomo Nieminen, Antti Onnela, Eva Partoll, Monica Passananti, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti P. Rissanen, Clémence Rose, Siegfried Schobesberger, Wiebke Scholz, Kay Scholze, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, Miguel Vazquez-Pufleau, Annele Virtanen, Alexander L. Vogel, Rainer Volkamer, Robert Wagner, Mingyi Wang, Lena Weitz, Daniela Wimmer, Mao Xiao, Chao Yan, Penglin Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Urs Baltensperger, Armin Hansel, Markku Kulmala, António Tomé, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 11809–11821, https://doi.org/10.5194/acp-20-11809-2020, https://doi.org/10.5194/acp-20-11809-2020, 2020
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With experiments performed at CLOUD, we show how isoprene interferes in monoterpene oxidation via RO2 termination at atmospherically relevant concentrations. This interference shifts the distribution of highly oxygenated organic molecules (HOMs) away from C20 class dimers towards C15 class dimers, which subsequently reduces both biogenic nucleation and early growth rates. Our results may help to understand the absence of new-particle formation in isoprene-rich environments.
Olli-Pekka Tikkanen, Angela Buchholz, Arttu Ylisirniö, Siegfried Schobesberger, Annele Virtanen, and Taina Yli-Juuti
Atmos. Chem. Phys., 20, 10441–10458, https://doi.org/10.5194/acp-20-10441-2020, https://doi.org/10.5194/acp-20-10441-2020, 2020
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We compared the volatility distributions of secondary organic aerosol (SOA) constituents estimated from isothermal evaporation experiments from either particle size change data, by process modelling and global optimization, or from mass spectrometer data with positive matrix factorization analysis. Our results show that, despite the two very different estimation methods, the volatility distributions are comparable if uncertainties are taken into account.
Petroc D. Shelley, Thomas J. Bannan, Stephen D. Worrall, M. Rami Alfarra, Ulrich K. Krieger, Carl J. Percival, Arthur Garforth, and David Topping
Atmos. Chem. Phys., 20, 8293–8314, https://doi.org/10.5194/acp-20-8293-2020, https://doi.org/10.5194/acp-20-8293-2020, 2020
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The methods used to estimate the vapour pressures of compounds in the atmosphere typically perform poorly when applied to organic compounds found in the atmosphere. New measurements have been made and compared to previous experimental data and estimated values so that the limitations within the estimation methods can be identified and in the future be rectified.
Angela Buchholz, Arttu Ylisirniö, Wei Huang, Claudia Mohr, Manjula Canagaratna, Douglas R. Worsnop, Siegfried Schobesberger, and Annele Virtanen
Atmos. Chem. Phys., 20, 7693–7716, https://doi.org/10.5194/acp-20-7693-2020, https://doi.org/10.5194/acp-20-7693-2020, 2020
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To understand the role of aerosol particles in the atmosphere, it is necessary to know their detailed chemical composition and physical properties, especially volatility. The thermal desorption data from FIGAERO–CIMS provides both but are difficult to analyse. With positive matrix factorisation, we can separate instrument background from the real signal. Compounds can be classified by their apparent volatility, and the contribution of thermal decomposition in the instrument can be identified.
Sini Isokääntä, Eetu Kari, Angela Buchholz, Liqing Hao, Siegfried Schobesberger, Annele Virtanen, and Santtu Mikkonen
Atmos. Meas. Tech., 13, 2995–3022, https://doi.org/10.5194/amt-13-2995-2020, https://doi.org/10.5194/amt-13-2995-2020, 2020
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Online mass spectrometry produces large amounts of data. These data can be interpreted with statistical methods, enabling scientists to more easily understand the underlying processes. We compared these techniques on car exhaust measurements. We show differences and similarities between the methods and give recommendations on applicability of the methods on certain types of data. We show that applying multiple methods leads to more robust results, thus increasing reliability of the findings.
Arttu Ylisirniö, Angela Buchholz, Claudia Mohr, Zijun Li, Luis Barreira, Andrew Lambe, Celia Faiola, Eetu Kari, Taina Yli-Juuti, Sergey A. Nizkorodov, Douglas R. Worsnop, Annele Virtanen, and Siegfried Schobesberger
Atmos. Chem. Phys., 20, 5629–5644, https://doi.org/10.5194/acp-20-5629-2020, https://doi.org/10.5194/acp-20-5629-2020, 2020
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We studied the chemical composition and volatility of secondary organic aerosol (SOA) particles formed from emissions of Scots pines and compared those results to SOA formed from α-pinene and from a sesquiterpene mixture. We found that SOA formed from single precursors cannot capture the properties of SOA formed from real plant emissions.
Kimmo Korhonen, Thomas Bjerring Kristensen, John Falk, Robert Lindgren, Christina Andersen, Ricardo Luis Carvalho, Vilhelm Malmborg, Axel Eriksson, Christoffer Boman, Joakim Pagels, Birgitta Svenningsson, Mika Komppula, Kari E. J. Lehtinen, and Annele Virtanen
Atmos. Chem. Phys., 20, 4951–4968, https://doi.org/10.5194/acp-20-4951-2020, https://doi.org/10.5194/acp-20-4951-2020, 2020
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Ice-nucleating abilities of particulate emissions from solid-fuel-burning cookstoves were studied using a portable ice nuclei counter in an extensive laboratory experiment campaign. We found that even small changes in combustion conditions may affect the ice-nucleating ability of the emissions significantly. Also six different physico-chemical properties of the emissions were studied, but no clear correlation to their ice-nucleating ability was found.
Gary Lloyd, Thomas Choularton, Keith Bower, Jonathan Crosier, Martin Gallagher, Michael Flynn, James Dorsey, Dantong Liu, Jonathan W. Taylor, Oliver Schlenczek, Jacob Fugal, Stephan Borrmann, Richard Cotton, Paul Field, and Alan Blyth
Atmos. Chem. Phys., 20, 3895–3904, https://doi.org/10.5194/acp-20-3895-2020, https://doi.org/10.5194/acp-20-3895-2020, 2020
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Measurements of liquid and ice cloud particles were made using an aircraft to penetrate fresh growing convective clouds in the tropical Atlantic. We found small ice particles at surprisingly high temperatures just below freezing. At colder temperatures secondary ice processes rapidly generated high concentrations of ice crystals.
Yu Wang, Ying Chen, Zhijun Wu, Dongjie Shang, Yuxuan Bian, Zhuofei Du, Sebastian H. Schmitt, Rong Su, Georgios I. Gkatzelis, Patrick Schlag, Thorsten Hohaus, Aristeidis Voliotis, Keding Lu, Limin Zeng, Chunsheng Zhao, M. Rami Alfarra, Gordon McFiggans, Alfred Wiedensohler, Astrid Kiendler-Scharr, Yuanhang Zhang, and Min Hu
Atmos. Chem. Phys., 20, 2161–2175, https://doi.org/10.5194/acp-20-2161-2020, https://doi.org/10.5194/acp-20-2161-2020, 2020
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Severe haze events, with high particulate nitrate (pNO3−) burden, frequently prevail in Beijing. In this study, we demonstrate a mutual-promotion effect between aerosol water uptake and pNO3− formation backed up by theoretical calculations and field observations throughout a typical pNO3−-dominated haze event in Beijing wintertime. This self-amplified mutual-promotion effect between aerosol water content and particulate nitrate can rapidly deteriorate air quality and degrade visibility.
Kathryn Fowler, Paul Connolly, and David Topping
Atmos. Chem. Phys., 20, 683–698, https://doi.org/10.5194/acp-20-683-2020, https://doi.org/10.5194/acp-20-683-2020, 2020
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Observations of low–temperature cirrus clouds have found unexpectedly low ice crystal numbers and high supersaturations, suggesting an incomplete understanding of the freezing mechanisms under these conditions. The existence of viscous organic aerosol has offered alternative ice nucleation pathways, which have been observed in laboratory studies. We have developed the first cloud parcel model to investigate the effect of viscosity on ice nucleation.
Olga Garmash, Matti P. Rissanen, Iida Pullinen, Sebastian Schmitt, Oskari Kausiala, Ralf Tillmann, Defeng Zhao, Carl Percival, Thomas J. Bannan, Michael Priestley, Åsa M. Hallquist, Einhard Kleist, Astrid Kiendler-Scharr, Mattias Hallquist, Torsten Berndt, Gordon McFiggans, Jürgen Wildt, Thomas F. Mentel, and Mikael Ehn
Atmos. Chem. Phys., 20, 515–537, https://doi.org/10.5194/acp-20-515-2020, https://doi.org/10.5194/acp-20-515-2020, 2020
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Highly oxygenated organic molecules (HOMs) facilitate aerosol formation in the atmosphere. Using NO3− chemical ionization mass spectrometry we investigated HOM composition and yield in oxidation of aromatic compounds at different reactant concentrations, in the presence of NOx and seed aerosol. Higher OH concentrations increased HOM yield, suggesting multiple oxidation steps, and affected HOM composition, potentially explaining in part discrepancies in published secondary organic aerosol yields.
Ying Chen, Oliver Wild, Edmund Ryan, Saroj Kumar Sahu, Douglas Lowe, Scott Archer-Nicholls, Yu Wang, Gordon McFiggans, Tabish Ansari, Vikas Singh, Ranjeet S. Sokhi, Alex Archibald, and Gufran Beig
Atmos. Chem. Phys., 20, 499–514, https://doi.org/10.5194/acp-20-499-2020, https://doi.org/10.5194/acp-20-499-2020, 2020
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PM2.5 and O3 are two major air pollutants. Some mitigation strategies focusing on reducing PM2.5 may lead to substantial increase in O3. We use statistical emulation combined with atmospheric transport model to perform thousands of sensitivity numerical studies to identify the major sources of PM2.5 and O3 and to develop strategies targeted at both pollutants. Our scientific evidence suggests that regional coordinated emission control is required to mitigate PM2.5 whilst preventing O3 increase.
Eetu Kari, Liqing Hao, Arttu Ylisirniö, Angela Buchholz, Ari Leskinen, Pasi Yli-Pirilä, Ilpo Nuutinen, Kari Kuuspalo, Jorma Jokiniemi, Celia L. Faiola, Siegfried Schobesberger, and Annele Virtanen
Atmos. Chem. Phys., 19, 15651–15671, https://doi.org/10.5194/acp-19-15651-2019, https://doi.org/10.5194/acp-19-15651-2019, 2019
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We present, for the first time, the dual effect of GDI-vehicle exhaust on α-pinene SOA mass yield suppression. The first effect is a well-known NOx effect, but the second effect is more complex. Our results imply that this second effect is related to change of reaction pathways of α-pinene in the presence of GDI exhaust. The presence of vehicle exhaust caused more than 50 % suppression in α-pinene SOA mass yield compared to the α-pinene SOA mass yield measured in the absence of GDI emissions.
Jianhui Jiang, Sebnem Aksoyoglu, Imad El-Haddad, Giancarlo Ciarelli, Hugo A. C. Denier van der Gon, Francesco Canonaco, Stefania Gilardoni, Marco Paglione, María Cruz Minguillón, Olivier Favez, Yunjiang Zhang, Nicolas Marchand, Liqing Hao, Annele Virtanen, Kalliopi Florou, Colin O'Dowd, Jurgita Ovadnevaite, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 19, 15247–15270, https://doi.org/10.5194/acp-19-15247-2019, https://doi.org/10.5194/acp-19-15247-2019, 2019
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We use an air quality model with a modified organic aerosol (OA) module based on chamber experiments to identify the OA sources and their contributions in Europe. Comparisons with long-term measurements at nine sites in 2011 show an improvement in OA simulation. Our results suggest that the biomass burning and biogenic emissions are the dominant sources in winter and summer, respectively. Contributions of diesel and gasoline vehicles are relatively small compared to a previous study in the US.
Jonathan W. Taylor, Sophie L. Haslett, Keith Bower, Michael Flynn, Ian Crawford, James Dorsey, Tom Choularton, Paul J. Connolly, Valerian Hahn, Christiane Voigt, Daniel Sauer, Régis Dupuy, Joel Brito, Alfons Schwarzenboeck, Thierry Bourriane, Cyrielle Denjean, Phil Rosenberg, Cyrille Flamant, James D. Lee, Adam R. Vaughan, Peter G. Hill, Barbara Brooks, Valéry Catoire, Peter Knippertz, and Hugh Coe
Atmos. Chem. Phys., 19, 8503–8522, https://doi.org/10.5194/acp-19-8503-2019, https://doi.org/10.5194/acp-19-8503-2019, 2019
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Low-level clouds cover a wide area of southern West Africa (SWA) and play an important role in the region's climate, reflecting sunlight away from the surface. We performed aircraft measurements of aerosols and clouds over SWA during the 2016 summer monsoon and found pollution, and polluted clouds, across the whole region. Smoke from biomass burning in Central Africa is transported to West Africa, causing a polluted background which limits the effect of local pollution on cloud properties.
Sebastian J. O'Shea, Jonathan Crosier, James Dorsey, Waldemar Schledewitz, Ian Crawford, Stephan Borrmann, Richard Cotton, and Aaron Bansemer
Atmos. Meas. Tech., 12, 3067–3079, https://doi.org/10.5194/amt-12-3067-2019, https://doi.org/10.5194/amt-12-3067-2019, 2019
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Optical array probe measurements of clouds are widely used to inform and validate numerical weather and climate models. In this paper, we discuss artefacts which may bias data from these instruments. Using laboratory and synthetic datasets, we demonstrate how greyscale analysis can be used to filter data, constraining the sample volume and improving data quality particularly at small sizes where their measurements are considered unreliable.
Zongbo Shi, Tuan Vu, Simone Kotthaus, Roy M. Harrison, Sue Grimmond, Siyao Yue, Tong Zhu, James Lee, Yiqun Han, Matthias Demuzere, Rachel E. Dunmore, Lujie Ren, Di Liu, Yuanlin Wang, Oliver Wild, James Allan, W. Joe Acton, Janet Barlow, Benjamin Barratt, David Beddows, William J. Bloss, Giulia Calzolai, David Carruthers, David C. Carslaw, Queenie Chan, Lia Chatzidiakou, Yang Chen, Leigh Crilley, Hugh Coe, Tie Dai, Ruth Doherty, Fengkui Duan, Pingqing Fu, Baozhu Ge, Maofa Ge, Daobo Guan, Jacqueline F. Hamilton, Kebin He, Mathew Heal, Dwayne Heard, C. Nicholas Hewitt, Michael Hollaway, Min Hu, Dongsheng Ji, Xujiang Jiang, Rod Jones, Markus Kalberer, Frank J. Kelly, Louisa Kramer, Ben Langford, Chun Lin, Alastair C. Lewis, Jie Li, Weijun Li, Huan Liu, Junfeng Liu, Miranda Loh, Keding Lu, Franco Lucarelli, Graham Mann, Gordon McFiggans, Mark R. Miller, Graham Mills, Paul Monk, Eiko Nemitz, Fionna O'Connor, Bin Ouyang, Paul I. Palmer, Carl Percival, Olalekan Popoola, Claire Reeves, Andrew R. Rickard, Longyi Shao, Guangyu Shi, Dominick Spracklen, David Stevenson, Yele Sun, Zhiwei Sun, Shu Tao, Shengrui Tong, Qingqing Wang, Wenhua Wang, Xinming Wang, Xuejun Wang, Zifang Wang, Lianfang Wei, Lisa Whalley, Xuefang Wu, Zhijun Wu, Pinhua Xie, Fumo Yang, Qiang Zhang, Yanli Zhang, Yuanhang Zhang, and Mei Zheng
Atmos. Chem. Phys., 19, 7519–7546, https://doi.org/10.5194/acp-19-7519-2019, https://doi.org/10.5194/acp-19-7519-2019, 2019
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APHH-Beijing is a collaborative international research programme to study the sources, processes and health effects of air pollution in Beijing. This introduction to the special issue provides an overview of (i) the APHH-Beijing programme, (ii) the measurement and modelling activities performed as part of it and (iii) the air quality and meteorological conditions during joint intensive field campaigns as a core activity within APHH-Beijing.
Eoghan Darbyshire, William T. Morgan, James D. Allan, Dantong Liu, Michael J. Flynn, James R. Dorsey, Sebastian J. O'Shea, Douglas Lowe, Kate Szpek, Franco Marenco, Ben T. Johnson, Stephane Bauguitte, Jim M. Haywood, Joel F. Brito, Paulo Artaxo, Karla M. Longo, and Hugh Coe
Atmos. Chem. Phys., 19, 5771–5790, https://doi.org/10.5194/acp-19-5771-2019, https://doi.org/10.5194/acp-19-5771-2019, 2019
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A novel analysis of aerosol and gas-phase vertical profiles shows a marked regional pollution contrast: composition is driven by the fire regime and vertical distribution is driven by thermodynamics. These drivers ought to be well represented in simulations to ensure realistic prediction of climate and air quality impacts. The BC : CO ratio in haze and plumes increases with altitude – long-range transport or fire stage coupled to plume dynamics may be responsible. Further enquiry is advocated.
Angela Buchholz, Andrew T. Lambe, Arttu Ylisirniö, Zijun Li, Olli-Pekka Tikkanen, Celia Faiola, Eetu Kari, Liqing Hao, Olli Luoma, Wei Huang, Claudia Mohr, Douglas R. Worsnop, Sergey A. Nizkorodov, Taina Yli-Juuti, Siegfried Schobesberger, and Annele Virtanen
Atmos. Chem. Phys., 19, 4061–4073, https://doi.org/10.5194/acp-19-4061-2019, https://doi.org/10.5194/acp-19-4061-2019, 2019
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We studied the evaporation of α-pinene secondary organic aerosol particles in clean air to derive their volatility from the observed size changes. We found that the particles became more resilient to evaporation with increased oxidative age, possibly increasing their lifetime in the atmosphere. Also, increased relative humidity increased the particle evaporation. Mass spectrometry measurements of the particles at different stages of evaporation revealed some water-induced composition changes.
Thomas J. Bannan, Michael Le Breton, Michael Priestley, Stephen D. Worrall, Asan Bacak, Nicholas A. Marsden, Archit Mehra, Julia Hammes, Mattias Hallquist, M. Rami Alfarra, Ulrich K. Krieger, Jonathan P. Reid, John Jayne, Wade Robinson, Gordon McFiggans, Hugh Coe, Carl J. Percival, and Dave Topping
Atmos. Meas. Tech., 12, 1429–1439, https://doi.org/10.5194/amt-12-1429-2019, https://doi.org/10.5194/amt-12-1429-2019, 2019
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The Filter Inlet for Gases and AEROsols (FIGAERO) is an inlet designed to be coupled with a high-resolution time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) and provides simultaneous molecular information relating to both the gas- and particle-phase samples. This method has been used to extract vapour pressures of compounds whilst giving quantitative concentrations in the particle phase. Here we detail an ideal set of benchmark compounds for characterization of the FIGAERO.
Liqing Hao, Olga Garmash, Mikael Ehn, Pasi Miettinen, Paola Massoli, Santtu Mikkonen, Tuija Jokinen, Pontus Roldin, Pasi Aalto, Taina Yli-Juuti, Jorma Joutsensaari, Tuukka Petäjä, Markku Kulmala, Kari E. J. Lehtinen, Douglas R. Worsnop, and Annele Virtanen
Atmos. Chem. Phys., 18, 17705–17716, https://doi.org/10.5194/acp-18-17705-2018, https://doi.org/10.5194/acp-18-17705-2018, 2018
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An aerosol mass spectrometer was used to characterize aerosol chemical composition during new particle formation periods. The time profiles of mass concentrations and chemical composition of observed aerosol particles are subjected to joint effects of boundary layer dilution, atmospheric chemistry and aerosol mixing in different boundary layers. During the nighttime, the increase in organic aerosol mass correlated well with the increase in condensed highly oxygenated organic molecules' mass.
Dawei Hu, David Topping, and Gordon McFiggans
Atmos. Chem. Phys., 18, 14925–14937, https://doi.org/10.5194/acp-18-14925-2018, https://doi.org/10.5194/acp-18-14925-2018, 2018
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Co-condensation of inorganic or organic vapours on growing droplets could significantly enhance both CCN and cloud droplet number concentration, thereby influencing climate. Until now, there has been very few direct observational evidence of this process. We exposed involatile inorganic particles to a moist atmosphere containing a controlled amount of an organic semi-volatile vapour. We measured a much greater growth of the particles than if they had only been exposed to water vapour.
Tuomo Nieminen, Veli-Matti Kerminen, Tuukka Petäjä, Pasi P. Aalto, Mikhail Arshinov, Eija Asmi, Urs Baltensperger, David C. S. Beddows, Johan Paul Beukes, Don Collins, Aijun Ding, Roy M. Harrison, Bas Henzing, Rakesh Hooda, Min Hu, Urmas Hõrrak, Niku Kivekäs, Kaupo Komsaare, Radovan Krejci, Adam Kristensson, Lauri Laakso, Ari Laaksonen, W. Richard Leaitch, Heikki Lihavainen, Nikolaos Mihalopoulos, Zoltán Németh, Wei Nie, Colin O'Dowd, Imre Salma, Karine Sellegri, Birgitta Svenningsson, Erik Swietlicki, Peter Tunved, Vidmantas Ulevicius, Ville Vakkari, Marko Vana, Alfred Wiedensohler, Zhijun Wu, Annele Virtanen, and Markku Kulmala
Atmos. Chem. Phys., 18, 14737–14756, https://doi.org/10.5194/acp-18-14737-2018, https://doi.org/10.5194/acp-18-14737-2018, 2018
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Atmospheric aerosols have diverse effects on air quality, human health, and global climate. One important source of aerosols is their formation via nucleation and growth in the atmosphere. We have analyzed long-term observations of regional new particle formation events around the globe and provide a comprehensive view on the characteristics of this phenomenon in diverse environments. The results are useful in developing more realistic representation of atmospheric aerosols in global models.
Maryam Dalirian, Arttu Ylisirniö, Angela Buchholz, Daniel Schlesinger, Johan Ström, Annele Virtanen, and Ilona Riipinen
Atmos. Chem. Phys., 18, 12477–12489, https://doi.org/10.5194/acp-18-12477-2018, https://doi.org/10.5194/acp-18-12477-2018, 2018
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Atmospheric black carbon (BC) particles are a concern due to their impact on air quality and climate. Their net climate effect is, however, still uncertain. In this study, laboratory measurements were performed to investigate cloud condensation nuclei (CCN) activity of BC particles, in pure state or coated by various organic species. Our results show that existing theories have potential in describing the CCN activation of atmospheric BC mixed with soluble pollutants.
Ben H. Lee, Felipe D. Lopez-Hilfiker, Emma L. D'Ambro, Putian Zhou, Michael Boy, Tuukka Petäjä, Liqing Hao, Annele Virtanen, and Joel A. Thornton
Atmos. Chem. Phys., 18, 11547–11562, https://doi.org/10.5194/acp-18-11547-2018, https://doi.org/10.5194/acp-18-11547-2018, 2018
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Molecular identities and abundances of organic compounds residing in the gas and particle phases above a Finnish boreal forest are presented. We determined that in each phase, the organic components are categorized into three subgroups based on their behavior in time. Some are more enhanced at night, others during midday, and another around sunrise. Identifying such collective behavior can potentially connect the chemical processes that evolve in time to specific distributions of products.
Matthew Crooks, Paul Connolly, and Gordon McFiggans
Geosci. Model Dev., 11, 3261–3278, https://doi.org/10.5194/gmd-11-3261-2018, https://doi.org/10.5194/gmd-11-3261-2018, 2018
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Clouds form when water condenses onto particles in the atmosphere and the size and chemical composition of these particles can have a large influence over how much water condenses and the subsequent formation of cloud. Additional gases exist in the atmosphere that can condense onto the aerosol particles and change their composition. We present a fast and efficient method of calculating the effect of atmospheric gases on the formation of cloud that can be used in climate and weather models.
Kelly L. Pereira, Rachel Dunmore, James Whitehead, M. Rami Alfarra, James D. Allan, Mohammed S. Alam, Roy M. Harrison, Gordon McFiggans, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 18, 11073–11096, https://doi.org/10.5194/acp-18-11073-2018, https://doi.org/10.5194/acp-18-11073-2018, 2018
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Exhaust emissions from a light-duty diesel engine were introduced into an atmospheric simulation chamber which was used as a holding-cell for sampling, allowing instruments capable of providing detailed chemical speciation of exhaust gas emissions to be used. The effect of different engine conditions on the exhaust gas composition was investigated. The exhaust composition changed considerably due to two influencing factors, engine combustion and diesel oxidative catalyst efficiency.
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.
Emma L. Simpson, Paul J. Connolly, and Gordon McFiggans
Atmos. Chem. Phys., 18, 7237–7250, https://doi.org/10.5194/acp-18-7237-2018, https://doi.org/10.5194/acp-18-7237-2018, 2018
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This study explores the process of ice formation in clouds by conducting computer model simulations and laboratory experiments in a cloud chamber. We show that the formation of ice in clouds can be limited by the presence of atmospheric aerosol particles and that further research is required to identify the requirements for freezing, e.g. minimum mass of water, in order to accurately calculate ice formation and thus improve climate and weather prediction.
Wei Huang, Harald Saathoff, Aki Pajunoja, Xiaoli Shen, Karl-Heinz Naumann, Robert Wagner, Annele Virtanen, Thomas Leisner, and Claudia Mohr
Atmos. Chem. Phys., 18, 2883–2898, https://doi.org/10.5194/acp-18-2883-2018, https://doi.org/10.5194/acp-18-2883-2018, 2018
Kathryn Fowler, Paul J. Connolly, David O. Topping, and Simon O'Meara
Atmos. Chem. Phys., 18, 1629–1642, https://doi.org/10.5194/acp-18-1629-2018, https://doi.org/10.5194/acp-18-1629-2018, 2018
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This is the first time the Maxwell–Stefan framework has been applied to an atmospheric aerosol core–shell model and shows that there is a complex interplay between the viscous and solubility effects on aerosol composition. Understanding aerosol composition is essential to accurately model their interactions within atmospheric systems. We use simple binary systems to demonstrate how viscosity and solubility both play a role in affecting the rate of diffusion through aerosol particles.
Gillian Young, Paul J. Connolly, Christopher Dearden, and Thomas W. Choularton
Atmos. Chem. Phys., 18, 1475–1494, https://doi.org/10.5194/acp-18-1475-2018, https://doi.org/10.5194/acp-18-1475-2018, 2018
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Large-scale subsidence, associated with high-pressure systems, is often used in cloud-resolving models to maintain the height of boundary layer clouds; however, its influence on the small-scale interactions in mixed-phase clouds has not been previously investigated. Using large-eddy simulations, we have identified a relationship between subsidence and convection development in such clouds, with implications for mixed-phase boundary layer clouds forming in the ocean-exposed Arctic regions.
Olivia Goulden, Matthew Crooks, and Paul Connolly
Atmos. Chem. Phys., 18, 275–287, https://doi.org/10.5194/acp-18-275-2018, https://doi.org/10.5194/acp-18-275-2018, 2018
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The formation of cloud from the condensation of water vapour in the atmosphere on aerosol particles is highly dependent of the chemical properties of the particles. The chemistry is further complicated by the presence of condensible gases in the atmosphere other than water. We provide several methods of including the complicated chemical properties of the aerosol particles and condensing gases into single parameter descriptions, which are suitable for inclusion in large-scale models.
Simon O'Meara, David O. Topping, Rahul A. Zaveri, and Gordon McFiggans
Atmos. Chem. Phys., 17, 10477–10494, https://doi.org/10.5194/acp-17-10477-2017, https://doi.org/10.5194/acp-17-10477-2017, 2017
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To simulate particle-phase diffusion, an analytical expression is desired because it takes less calculation time than a differential equation. Here a correction is found for the analytical solution for when diffusivity is dependent on composition, thereby making it more widely applicable than before. Consequently, we are able to more realistically evaluate the rate limitation (if any) imposed by particle-phase diffusion on component partitioning between the gas and particle phase.
Leonid Nichman, Emma Järvinen, James Dorsey, Paul Connolly, Jonathan Duplissy, Claudia Fuchs, Karoliina Ignatius, Kamalika Sengupta, Frank Stratmann, Ottmar Möhler, Martin Schnaiter, and Martin Gallagher
Atmos. Meas. Tech., 10, 3231–3248, https://doi.org/10.5194/amt-10-3231-2017, https://doi.org/10.5194/amt-10-3231-2017, 2017
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Optical probes are frequently used for the detection of cloud particles. The detected microphysical properties may affect particle growth and accretion mechanisms and the light scattering properties of cirrus clouds. In the CLOUD chamber study at CERN, we compared four optical measurement techniques. We show that shape derivation alone is not sufficient to determine the phase of the small cloud particles. None of the instruments were able to unambiguously determine the phase of small particles.
David O. Topping, James Allan, M. Rami Alfarra, and Bernard Aumont
Geosci. Model Dev., 10, 2365–2377, https://doi.org/10.5194/gmd-10-2365-2017, https://doi.org/10.5194/gmd-10-2365-2017, 2017
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Our ability to model the chemical and thermodynamic processes that lead to secondary organic aerosol (SOA) formation is thought to be hampered by the complexity of the system. In this proof of concept study, the ability to train supervised methods to predict electron impact ionisation (EI) mass spectra for the AMS is evaluated to facilitate improved model evaluation. The study demonstrates the use of a methodology that would be improved with more training data and data from simple mixed systems.
Huan Yao, Yu Song, Mingxu Liu, Scott Archer-Nicholls, Douglas Lowe, Gordon McFiggans, Tingting Xu, Pin Du, Jianfeng Li, Yusheng Wu, Min Hu, Chun Zhao, and Tong Zhu
Atmos. Chem. Phys., 17, 5205–5219, https://doi.org/10.5194/acp-17-5205-2017, https://doi.org/10.5194/acp-17-5205-2017, 2017
Juan Hong, Mikko Äijälä, Silja A. K. Häme, Liqing Hao, Jonathan Duplissy, Liine M. Heikkinen, Wei Nie, Jyri Mikkilä, Markku Kulmala, Nønne L. Prisle, Annele Virtanen, Mikael Ehn, Pauli Paasonen, Douglas R. Worsnop, Ilona Riipinen, Tuukka Petäjä, and Veli-Matti Kerminen
Atmos. Chem. Phys., 17, 4387–4399, https://doi.org/10.5194/acp-17-4387-2017, https://doi.org/10.5194/acp-17-4387-2017, 2017
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Estimates of volatility of secondary organic aerosols was characterized in a boreal forest environment of Hyytiälä, southern Finland. This was done by interpreting field measurements using a volatility tandem differential mobility analyzer (VTDMA) with a kinetic evaporation model and by applying positive matrix factorization (PMF) to high-resolution aerosol mass spectrometer data. About 16 % of the variation can be explained by the linear regression between the results from these two methods.
Gillian Young, Paul J. Connolly, Hazel M. Jones, and Thomas W. Choularton
Atmos. Chem. Phys., 17, 4209–4227, https://doi.org/10.5194/acp-17-4209-2017, https://doi.org/10.5194/acp-17-4209-2017, 2017
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Arctic mixed-phase clouds are poorly represented in numerical models, due in part to an overpredicted ice phase. Here, we examine the sensitivity of cloud structure, evolution, and lifetime to modelled primary ice number concentrations over three different surfaces – sea ice, marginal ice, and ocean – to investigate the dependency on both the ice phase and dynamics induced from surface fluxes.
Wei Nie, Juan Hong, Silja A. K. Häme, Aijun Ding, Yugen Li, Chao Yan, Liqing Hao, Jyri Mikkilä, Longfei Zheng, Yuning Xie, Caijun Zhu, Zheng Xu, Xuguang Chi, Xin Huang, Yang Zhou, Peng Lin, Annele Virtanen, Douglas R. Worsnop, Markku Kulmala, Mikael Ehn, Jianzhen Yu, Veli-Matti Kerminen, and Tuukka Petäjä
Atmos. Chem. Phys., 17, 3659–3672, https://doi.org/10.5194/acp-17-3659-2017, https://doi.org/10.5194/acp-17-3659-2017, 2017
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HULIS are demonstrated to be important low-volatility, or even extremely low volatility, compounds in the organic aerosol phase. This sheds new light on the connection between atmospheric HULIS and ELVOCs. The interaction between HULIS and ammonium sulfate was found to decrease the volatility of the HULIS part in HULIS-AS mixed samples, indicating multiphase processes have the potential to lower the volatility of organic compounds in the aerosol phase.
Gillian Young, Hazel M. Jones, Thomas W. Choularton, Jonathan Crosier, Keith N. Bower, Martin W. Gallagher, Rhiannon S. Davies, Ian A. Renfrew, Andrew D. Elvidge, Eoghan Darbyshire, Franco Marenco, Philip R. A. Brown, Hugo M. A. Ricketts, Paul J. Connolly, Gary Lloyd, Paul I. Williams, James D. Allan, Jonathan W. Taylor, Dantong Liu, and Michael J. Flynn
Atmos. Chem. Phys., 16, 13945–13967, https://doi.org/10.5194/acp-16-13945-2016, https://doi.org/10.5194/acp-16-13945-2016, 2016
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Clouds are intricately coupled to the Arctic sea ice. Our inability to accurately model cloud fractions causes large uncertainties in predicted radiative interactions in this region, therefore, affecting sea ice forecasts. Here, we present measurements of cloud microphysics, aerosol properties, and thermodynamic structure over the transition from sea ice to ocean to improve our understanding of the relationship between the Arctic atmosphere and clouds which develop in this region.
Michael J. Lawler, Paul M. Winkler, Jaeseok Kim, Lars Ahlm, Jasmin Tröstl, Arnaud P. Praplan, Siegfried Schobesberger, Andreas Kürten, Jasper Kirkby, Federico Bianchi, Jonathan Duplissy, Armin Hansel, Tuija Jokinen, Helmi Keskinen, Katrianne Lehtipalo, Markus Leiminger, Tuukka Petäjä, Matti Rissanen, Linda Rondo, Mario Simon, Mikko Sipilä, Christina Williamson, Daniela Wimmer, Ilona Riipinen, Annele Virtanen, and James N. Smith
Atmos. Chem. Phys., 16, 13601–13618, https://doi.org/10.5194/acp-16-13601-2016, https://doi.org/10.5194/acp-16-13601-2016, 2016
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We present chemical observations of newly formed particles as small as ~ 10 nm from new particle formation experiments using sulfuric acid, dimethylamine, ammonia, and water vapor as gas phase reactants. The nanoparticles were more acidic than expected based on thermodynamic expectations, particularly at the smallest measured sizes. The results suggest rapid surface conversion of SO2 to sulfate and show a marked composition change between 10 and 15 nm, possibly indicating a phase change.
François Benduhn, Graham W. Mann, Kirsty J. Pringle, David O. Topping, Gordon McFiggans, and Kenneth S. Carslaw
Geosci. Model Dev., 9, 3875–3906, https://doi.org/10.5194/gmd-9-3875-2016, https://doi.org/10.5194/gmd-9-3875-2016, 2016
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We present a new mathematical formalism that serves to represent exchanges of inorganic matter between the atmosphere gas phase and the aerosol aqueous phase. In a global modelling framework, taking into account these processes may help represent many important features more accurately, such as the formation of cloud droplets or the radiative properties of the atmosphere. The formalism strives to keep an appropriate balance between accuracy and computation efficiency requirements.
Petri Tiitta, Ari Leskinen, Liqing Hao, Pasi Yli-Pirilä, Miika Kortelainen, Julija Grigonyte, Jarkko Tissari, Heikki Lamberg, Anni Hartikainen, Kari Kuuspalo, Aki-Matti Kortelainen, Annele Virtanen, Kari E. J. Lehtinen, Mika Komppula, Simone Pieber, André S. H. Prévôt, Timothy B. Onasch, Douglas R. Worsnop, Hendryk Czech, Ralf Zimmermann, Jorma Jokiniemi, and Olli Sippula
Atmos. Chem. Phys., 16, 13251–13269, https://doi.org/10.5194/acp-16-13251-2016, https://doi.org/10.5194/acp-16-13251-2016, 2016
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Real-time measurements of OA aging and SOA formation from logwood combustion were conducted under dark and UV oxidation. Substantial SOA formation was observed in all experiments, leading to twice the initial OA mass emphasizing the importance of the burning conditions for the aging processes. The results prove that emissions are subject to intensive chemical processing in the atmosphere; e.g. the most of the POA was found to become oxidized after the ozone addition, forming aged POA.
Matthew Crooks, Paul Connolly, David Topping, and Gordon McFiggans
Geosci. Model Dev., 9, 3617–3637, https://doi.org/10.5194/gmd-9-3617-2016, https://doi.org/10.5194/gmd-9-3617-2016, 2016
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Semi-volatile compounds, like water, can exist in both vapour phases and condensed phases within a system. This paper presents a method of calculating the condensed and vapour phases of semi-volatile compounds at equilibrium, in particular, when the condensed mass occurs within particles of different sizes and chemical composition. The applications of interest to the authors are those of atmospheric importance such as cloud droplet formation and reflection or absorption of solar radiation.
Valery Shcherbakov, Olivier Jourdan, Christiane Voigt, Jean-Francois Gayet, Aurélien Chauvigne, Alfons Schwarzenboeck, Andreas Minikin, Marcus Klingebiel, Ralf Weigel, Stephan Borrmann, Tina Jurkat, Stefan Kaufmann, Romy Schlage, Christophe Gourbeyre, Guy Febvre, Tatyana Lapyonok, Wiebke Frey, Sergej Molleker, and Bernadett Weinzierl
Atmos. Chem. Phys., 16, 11883–11897, https://doi.org/10.5194/acp-16-11883-2016, https://doi.org/10.5194/acp-16-11883-2016, 2016
Aki Pajunoja, Weiwei Hu, Yu J. Leong, Nathan F. Taylor, Pasi Miettinen, Brett B. Palm, Santtu Mikkonen, Don R. Collins, Jose L. Jimenez, and Annele Virtanen
Atmos. Chem. Phys., 16, 11163–11176, https://doi.org/10.5194/acp-16-11163-2016, https://doi.org/10.5194/acp-16-11163-2016, 2016
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The phase state of ambient particles was inferred from bounce measurements conducted at a rural site in central Alabama during the SOAS campaign. The organic-dominated ambient particles are mostly in the liquid phase at summertime conditions but they turn semisolid when dried in the measurement setup. Bounce humidograms reveal that the hygroscopicity and oxidation of the particles decreases the liquefying RH. The effect of oxidation is emphasized by oxidation flow reactor measurements.
Olli Väisänen, Antti Ruuskanen, Arttu Ylisirniö, Pasi Miettinen, Harri Portin, Liqing Hao, Ari Leskinen, Mika Komppula, Sami Romakkaniemi, Kari E. J. Lehtinen, and Annele Virtanen
Atmos. Chem. Phys., 16, 10385–10398, https://doi.org/10.5194/acp-16-10385-2016, https://doi.org/10.5194/acp-16-10385-2016, 2016
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In-cloud measurements of aerosol hygroscopicity and cloud droplet activation were conducted in Kuopio, Finland. According to the observations, the less hygroscopic accumulation mode particles were present in the non-activated aerosol, whereas the more hygroscopic particles were scavenged into cloud droplets. The results illustrate the sensitivity of cloud droplet formation to varying chemical composition and highlight the need for proper treatment of anthropogenic aerosols in CCN predictions.
James D. Whitehead, Eoghan Darbyshire, Joel Brito, Henrique M. J. Barbosa, Ian Crawford, Rafael Stern, Martin W. Gallagher, Paul H. Kaye, James D. Allan, Hugh Coe, Paulo Artaxo, and Gordon McFiggans
Atmos. Chem. Phys., 16, 9727–9743, https://doi.org/10.5194/acp-16-9727-2016, https://doi.org/10.5194/acp-16-9727-2016, 2016
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We present measurements of aerosols during the transition from wet to dry seasons at a pristine rainforest site in central Amazonia. By excluding pollution episodes, we focus on natural biogenic aerosols. Submicron aerosols are dominated by organic material, similar to previous wet season measurements. Larger particles are dominated by biological material, mostly fungal spores, with higher concentrations at night. This study provides important data on the nature of particles above the Amazon.
Bernadette Rosati, Martin Gysel, Florian Rubach, Thomas F. Mentel, Brigitta Goger, Laurent Poulain, Patrick Schlag, Pasi Miettinen, Aki Pajunoja, Annele Virtanen, Henk Klein Baltink, J. S. Bas Henzing, Johannes Größ, Gian Paolo Gobbi, Alfred Wiedensohler, Astrid Kiendler-Scharr, Stefano Decesari, Maria Cristina Facchini, Ernest Weingartner, and Urs Baltensperger
Atmos. Chem. Phys., 16, 7295–7315, https://doi.org/10.5194/acp-16-7295-2016, https://doi.org/10.5194/acp-16-7295-2016, 2016
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This study presents PEGASOS project data from field campaigns in the Po Valley, Italy and the Netherlands. Vertical profiles of aerosol hygroscopicity and chemical composition were investigated with airborne measurements on board a Zeppelin NT airship. A special focus was on the evolution of different mixing layers within the PBL as a function of daytime. A closure study showed that variations in aerosol hygroscopicity can well be explained by the variations in chemical composition.
Karoliina Ignatius, Thomas B. Kristensen, Emma Järvinen, Leonid Nichman, Claudia Fuchs, Hamish Gordon, Paul Herenz, Christopher R. Hoyle, Jonathan Duplissy, Sarvesh Garimella, Antonio Dias, Carla Frege, Niko Höppel, Jasmin Tröstl, Robert Wagner, Chao Yan, Antonio Amorim, Urs Baltensperger, Joachim Curtius, Neil M. Donahue, Martin W. Gallagher, Jasper Kirkby, Markku Kulmala, Ottmar Möhler, Harald Saathoff, Martin Schnaiter, Antonio Tomé, Annele Virtanen, Douglas Worsnop, and Frank Stratmann
Atmos. Chem. Phys., 16, 6495–6509, https://doi.org/10.5194/acp-16-6495-2016, https://doi.org/10.5194/acp-16-6495-2016, 2016
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Viscous solid or semi-solid secondary organic aerosol (SOA) may influence cloud properties through ice nucleation in the atmosphere. Here, we observed heterogeneous ice nucleation of viscous α-pinene SOA at temperatures between −39 °C and −37.2 °C with ice saturation ratios significantly below the homogeneous freezing limit. Global modelling suggests that viscous biogenic SOA are present in regions where cirrus formation takes place and could contribute to the global ice nuclei budget.
Scott Archer-Nicholls, Douglas Lowe, David M. Schultz, and Gordon McFiggans
Atmos. Chem. Phys., 16, 5573–5594, https://doi.org/10.5194/acp-16-5573-2016, https://doi.org/10.5194/acp-16-5573-2016, 2016
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The response of the Weather Research and Forecasting model with Chemistry to forcings by biomass burning aerosol were investigated in high-resolution nested domains over Brazil. The aerosol-layer was found to have a negative direct effect at the top of the atmosphere, but this was largely cancelled by a semi-direct effect which inhibited afternoon cloud formation. The cloud response to the aerosol was found to be highly sensitive to model resolution and the use of convective parameterisation.
Simon O'Meara, David O. Topping, and Gordon McFiggans
Atmos. Chem. Phys., 16, 5299–5313, https://doi.org/10.5194/acp-16-5299-2016, https://doi.org/10.5194/acp-16-5299-2016, 2016
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To understand the effect of atmospheric particulate matter on climate and human health we need to know how it evolves. We investigate how best to estimate diffusion of components through particles by comparing diffusion times from three approaches to solving Fick's Law and find that they agree. This means that scientists can simulate Fickian diffusion through atmospheric particles using the approach best suited to their requirements and have confidence that their model is mathematically sound.
Robert J. Farrington, Paul J. Connolly, Gary Lloyd, Keith N. Bower, Michael J. Flynn, Martin W. Gallagher, Paul R. Field, Chris Dearden, and Thomas W. Choularton
Atmos. Chem. Phys., 16, 4945–4966, https://doi.org/10.5194/acp-16-4945-2016, https://doi.org/10.5194/acp-16-4945-2016, 2016
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This paper assesses the reasons for high ice number concentrations observed in orographic clouds by comparing observations with model simulations over Jungfraujoch, Switzerland. The results suggest that ice nuclei do not significantly contribute to the high concentrations and that a surface source of ice crystals is responsible for the witnessed ice number concentrations.
Bernadette Rosati, Erik Herrmann, Silvia Bucci, Federico Fierli, Francesco Cairo, Martin Gysel, Ralf Tillmann, Johannes Größ, Gian Paolo Gobbi, Luca Di Liberto, Guido Di Donfrancesco, Alfred Wiedensohler, Ernest Weingartner, Annele Virtanen, Thomas F. Mentel, and Urs Baltensperger
Atmos. Chem. Phys., 16, 4539–4554, https://doi.org/10.5194/acp-16-4539-2016, https://doi.org/10.5194/acp-16-4539-2016, 2016
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We present vertical profiles of aerosol optical properties, which were explored within the planetary boundary layer in a case study in 2012 in the Po Valley region. A comparison of in situ measurements recorded aboard a Zeppelin NT and ground-based remote-sensing data was performed yielding good agreement. Additionally, the role of ambient relative humidity for the aerosol particles' optical properties was investigated.
Emma Järvinen, Karoliina Ignatius, Leonid Nichman, Thomas B. Kristensen, Claudia Fuchs, Christopher R. Hoyle, Niko Höppel, Joel C. Corbin, Jill Craven, Jonathan Duplissy, Sebastian Ehrhart, Imad El Haddad, Carla Frege, Hamish Gordon, Tuija Jokinen, Peter Kallinger, Jasper Kirkby, Alexei Kiselev, Karl-Heinz Naumann, Tuukka Petäjä, Tamara Pinterich, Andre S. H. Prevot, Harald Saathoff, Thea Schiebel, Kamalika Sengupta, Mario Simon, Jay G. Slowik, Jasmin Tröstl, Annele Virtanen, Paul Vochezer, Steffen Vogt, Andrea C. Wagner, Robert Wagner, Christina Williamson, Paul M. Winkler, Chao Yan, Urs Baltensperger, Neil M. Donahue, Rick C. Flagan, Martin Gallagher, Armin Hansel, Markku Kulmala, Frank Stratmann, Douglas R. Worsnop, Ottmar Möhler, Thomas Leisner, and Martin Schnaiter
Atmos. Chem. Phys., 16, 4423–4438, https://doi.org/10.5194/acp-16-4423-2016, https://doi.org/10.5194/acp-16-4423-2016, 2016
G. Young, H. M. Jones, E. Darbyshire, K. J. Baustian, J. B. McQuaid, K. N. Bower, P. J. Connolly, M. W. Gallagher, and T. W. Choularton
Atmos. Chem. Phys., 16, 4063–4079, https://doi.org/10.5194/acp-16-4063-2016, https://doi.org/10.5194/acp-16-4063-2016, 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
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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.
David Topping, Mark Barley, Michael K. Bane, Nicholas Higham, Bernard Aumont, Nicholas Dingle, and Gordon McFiggans
Geosci. Model Dev., 9, 899–914, https://doi.org/10.5194/gmd-9-899-2016, https://doi.org/10.5194/gmd-9-899-2016, 2016
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In this paper we describe the development and application of a new web-based and open-source facility, UManSysProp (http://umansysprop .seaes.manchester.ac.uk), for automating predictions of molecular and atmospheric aerosol properties. Current facilities include pure component vapour pressures, critical properties, and sub-cooled densities of organic molecules; activity coefficient predictions for mixed inorganic-organic liquid systems; hygroscopic growth factors and CCN activation potential.
I. Crawford, G. Lloyd, E. Herrmann, C. R. Hoyle, K. N. Bower, P. J. Connolly, M. J. Flynn, P. H. Kaye, T. W. Choularton, and M. W. Gallagher
Atmos. Chem. Phys., 16, 2273–2284, https://doi.org/10.5194/acp-16-2273-2016, https://doi.org/10.5194/acp-16-2273-2016, 2016
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In this manuscript we discuss observations of fluorescent aerosol and their interactions with cloud at a high-alpine site in the wintertime under background conditions. We find the majority of the fluorescent aerosol to be consistent in nature to mineral dust and no apparent trend was observed between the fluorescent aerosol fraction and meteorological or cloud microphysical parameters, suggesting that particle fluorescence does not impact cloud evolution or formation at the site.
J. Kim, L. Ahlm, T. Yli-Juuti, M. Lawler, H. Keskinen, J. Tröstl, S. Schobesberger, J. Duplissy, A. Amorim, F. Bianchi, N. M. Donahue, R. C. Flagan, J. Hakala, M. Heinritzi, T. Jokinen, A. Kürten, A. Laaksonen, K. Lehtipalo, P. Miettinen, T. Petäjä, M. P. Rissanen, L. Rondo, K. Sengupta, M. Simon, A. Tomé, C. Williamson, D. Wimmer, P. M. Winkler, S. Ehrhart, P. Ye, J. Kirkby, J. Curtius, U. Baltensperger, M. Kulmala, K. E. J. Lehtinen, J. N. Smith, I. Riipinen, and A. Virtanen
Atmos. Chem. Phys., 16, 293–304, https://doi.org/10.5194/acp-16-293-2016, https://doi.org/10.5194/acp-16-293-2016, 2016
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The hygroscopicity of nucleated nanoparticles was measured in the presence of sulfuric acid, sulfuric acid-dimethylamine, and sulfuric acid-organics derived from α-pinene oxidation during CLOUD7 at CERN in 2012. The hygroscopicity parameter κ decreased with increasing particle size, indicating decreasing acidity of particles.
A. M. K. Hansen, J. Hong, T. Raatikainen, K. Kristensen, A. Ylisirniö, A. Virtanen, T. Petäjä, M. Glasius, and N. L. Prisle
Atmos. Chem. Phys., 15, 14071–14089, https://doi.org/10.5194/acp-15-14071-2015, https://doi.org/10.5194/acp-15-14071-2015, 2015
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This paper presents the first study of the hygroscopic properties of limonene derived organosulfates (L-OS 250). The results showed that L-OS 250 particles are weakly hygroscopic and able to activate into cloud droplets. Particles of L-OS 250 mixed with ammonium sulfate were much more hygroscopic than expected from model parametrizations and the ZSR mixing rule, indicating that solubility and non-ideal droplet interactions could be important for the hygroscopic properties of the mixed particles.
J. Grazioli, G. Lloyd, L. Panziera, C. R. Hoyle, P. J. Connolly, J. Henneberger, and A. Berne
Atmos. Chem. Phys., 15, 13787–13802, https://doi.org/10.5194/acp-15-13787-2015, https://doi.org/10.5194/acp-15-13787-2015, 2015
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This study investigates the microphysics of winter alpine snowfall occurring in mixed-phase clouds in an inner-Alpine valley during CLACE2014. From polarimetric radar and in situ observations, riming is shown to be an important process leading to more intense snowfall. Riming is usually associated with more intense turbulence providing supercooled liquid water. Distinct features are identified in the vertical structure of polarimetric radar variables.
G. Lloyd, T. W. Choularton, K. N. Bower, M. W. Gallagher, P. J. Connolly, M. Flynn, R. Farrington, J. Crosier, O. Schlenczek, J. Fugal, and J. Henneberger
Atmos. Chem. Phys., 15, 12953–12969, https://doi.org/10.5194/acp-15-12953-2015, https://doi.org/10.5194/acp-15-12953-2015, 2015
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The paper explores the microphysical structure of clouds at the high-alpine measurement site Jungfraujoch, Switzerland. High concentrations of ice crystals were measured by a range of instruments. The presence of these high concentrations could not be explained through conventional understanding of ice formation processes in clouds and the possibility that the surface provides a significant source of ice crystals is investigated.
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. Hong, J. Kim, T. Nieminen, J. Duplissy, M. Ehn, M. Äijälä, L. Q. Hao, W. Nie, N. Sarnela, N. L. Prisle, M. Kulmala, A. Virtanen, T. Petäjä, and V.-M. Kerminen
Atmos. Chem. Phys., 15, 11999–12009, https://doi.org/10.5194/acp-15-11999-2015, https://doi.org/10.5194/acp-15-11999-2015, 2015
C. Emersic, P. J. Connolly, S. Boult, M. Campana, and Z. Li
Atmos. Chem. Phys., 15, 11311–11326, https://doi.org/10.5194/acp-15-11311-2015, https://doi.org/10.5194/acp-15-11311-2015, 2015
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K. P. Wyche, P. S. Monks, K. L. Smallbone, J. F. Hamilton, M. R. Alfarra, A. R. Rickard, G. B. McFiggans, M. E. Jenkin, W. J. Bloss, A. C. Ryan, C. N. Hewitt, and A. R. MacKenzie
Atmos. Chem. Phys., 15, 8077–8100, https://doi.org/10.5194/acp-15-8077-2015, https://doi.org/10.5194/acp-15-8077-2015, 2015
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This paper describes a new ensemble methodology for the statistical analysis of atmospheric gas- & particle-phase composition data sets. The methodology reduces the huge amount of data derived from many chamber experiments to show that organic reactivity & resultant particle formation can be mapped into unique clusters in statistical space. The model generated is used to map more realistic plant mesocosm oxidation data, the projection of which gives insight into reactive pathways & precursors.
W. Frey, R. Schofield, P. Hoor, D. Kunkel, F. Ravegnani, A. Ulanovsky, S. Viciani, F. D'Amato, and T. P. Lane
Atmos. Chem. Phys., 15, 6467–6486, https://doi.org/10.5194/acp-15-6467-2015, https://doi.org/10.5194/acp-15-6467-2015, 2015
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This study examines the simulated downward transport and mixing of stratospheric air into the upper tropical troposphere as observed on a research flight during the SCOUT-O3 campaign in connection with a deep convective system, using the WRF model. Passive tracers are initialised to study the impact of the deep convection on the tracers and water vapour. We use the model to explain the processes causing the transport and also expose areas of inconsistencies between the model and observations.
A. Leskinen, P. Yli-Pirilä, K. Kuuspalo, O. Sippula, P. Jalava, M.-R. Hirvonen, J. Jokiniemi, A. Virtanen, M. Komppula, and K. E. J. Lehtinen
Atmos. Meas. Tech., 8, 2267–2278, https://doi.org/10.5194/amt-8-2267-2015, https://doi.org/10.5194/amt-8-2267-2015, 2015
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A 29 m3 Teflon chamber was characterized and tested with oxidation experiments of toluene. Secondary organic aerosol yields of 12-42 % were obtained. These yields are comparable to those obtained in other laboratories.
J. D. Allan, P. I. Williams, J. Najera, J. D. Whitehead, M. J. Flynn, J. W. Taylor, D. Liu, E. Darbyshire, L. J. Carpenter, R. Chance, S. J. Andrews, S. C. Hackenberg, and G. McFiggans
Atmos. Chem. Phys., 15, 5599–5609, https://doi.org/10.5194/acp-15-5599-2015, https://doi.org/10.5194/acp-15-5599-2015, 2015
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New particle formation (NPF) is an important contributor to aerosol number concentrations in the Arctic and thus has a major role in dictating cloud properties and climate in this region. Here we present direct evidence that the oxidation of iodine in the atmosphere causes NPF in the Greenland Sea. This is important because this is a NPF mechanism that has not previously been considered in modelling studies at these latitudes.
M. Dalirian, H. Keskinen, L. Ahlm, A. Ylisirniö, S. Romakkaniemi, A. Laaksonen, A. Virtanen, and I. Riipinen
Atmos. Chem. Phys., 15, 3815–3829, https://doi.org/10.5194/acp-15-3815-2015, https://doi.org/10.5194/acp-15-3815-2015, 2015
I. Steinke, C. Hoose, O. Möhler, P. Connolly, and T. Leisner
Atmos. Chem. Phys., 15, 3703–3717, https://doi.org/10.5194/acp-15-3703-2015, https://doi.org/10.5194/acp-15-3703-2015, 2015
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Ice nucleation in clouds has a significant influence on the global radiative budget and the hydrological cycle. Several studies have investigated the ice formation in droplets and parameterizations have been developed in order to include immersion freezing in climate models. In contrast, there are fewer studies regarding the conversion of water vapor into ice (so-called deposition nucleation) which is the topic of this paper which investigates deposition nucleation by Arizona Test dust in detail
G. Lloyd, T. W. Choularton, K. N. Bower, J. Crosier, H. Jones, J. R. Dorsey, M. W. Gallagher, P. Connolly, A. C. R. Kirchgaessner, and T. Lachlan-Cope
Atmos. Chem. Phys., 15, 3719–3737, https://doi.org/10.5194/acp-15-3719-2015, https://doi.org/10.5194/acp-15-3719-2015, 2015
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Measurements of cloud microphysics are reported from the Aerosol-Cloud Coupling And Climate Interactions (ACCACIA) campaign. Concentrations of ice particles from two spring and two summer cases are compared with particular attention to the role of secondary ice in these clouds. In addition aerosol measurements were used as input to a primary ice nucleation parameterisation which was compared with observed values of primary ice in these clouds. We found higher concentrations of ice during summer.
M. D. Jolleys, H. Coe, G. McFiggans, J. W. Taylor, S. J. O'Shea, M. Le Breton, S. J.-B. Bauguitte, S. Moller, P. Di Carlo, E. Aruffo, P. I. Palmer, J. D. Lee, C. J. Percival, and M. W. Gallagher
Atmos. Chem. Phys., 15, 3077–3095, https://doi.org/10.5194/acp-15-3077-2015, https://doi.org/10.5194/acp-15-3077-2015, 2015
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Particulate emissions in the form of organic aerosol from boreal forest fires in Canada have been measured during an aircraft measurement campaign. Ratios of the amount of aerosol emitted relative to gas species such as CO were calculated and show high levels of variability throughout the campaign. This variability is affected by both changes in fire conditions, as fires tended to die down later in the measurement period, and by changes to the aerosol due to chemical reactions in the atmosphere.
S. Archer-Nicholls, D. Lowe, E. Darbyshire, W. T. Morgan, M. M. Bela, G. Pereira, J. Trembath, J. W. Kaiser, K. M. Longo, S. R. Freitas, H. Coe, and G. McFiggans
Geosci. Model Dev., 8, 549–577, https://doi.org/10.5194/gmd-8-549-2015, https://doi.org/10.5194/gmd-8-549-2015, 2015
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The regional WRF-Chem model was used to study aerosol particles from biomass burning in South America. The modelled estimates of fire plume injection heights were found to be too high, with serious implications for modelled aerosol vertical distribution, transport and impacts on local climate. A modified emission scenario was developed which improved the predicted injection height. Model results were compared and evaluated against in situ measurements from the 2012 SAMBBA flight campaign.
D. Lowe, S. Archer-Nicholls, W. Morgan, J. Allan, S. Utembe, B. Ouyang, E. Aruffo, M. Le Breton, R. A. Zaveri, P. Di Carlo, C. Percival, H. Coe, R. Jones, and G. McFiggans
Atmos. Chem. Phys., 15, 1385–1409, https://doi.org/10.5194/acp-15-1385-2015, https://doi.org/10.5194/acp-15-1385-2015, 2015
L. Q. Hao, A. Kortelainen, S. Romakkaniemi, H. Portin, A. Jaatinen, A. Leskinen, M. Komppula, P. Miettinen, D. Sueper, A. Pajunoja, J. N. Smith, K. E. J. Lehtinen, D. R. Worsnop, A. Laaksonen, and A. Virtanen
Atmos. Chem. Phys., 14, 13483–13495, https://doi.org/10.5194/acp-14-13483-2014, https://doi.org/10.5194/acp-14-13483-2014, 2014
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Positive matrix factorization (PMF) was applied to the unified high-resolution mass spectra organic species with NO+ and NO2+ ions from the measurement in a mixed region between the boreal forestland and the urban area. The PMF analysis succeeded in separating the mixed spectra into three distinct organic factors and one inorganic factor. The particulate organic nitrate was distinguished by PMF for the first time, with a contribution of one-third of the total nitrate mass.
W. Frey, S. Borrmann, F. Fierli, R. Weigel, V. Mitev, R. Matthey, F. Ravegnani, N. M. Sitnikov, A. Ulanovsky, and F. Cairo
Atmos. Chem. Phys., 14, 13223–13240, https://doi.org/10.5194/acp-14-13223-2014, https://doi.org/10.5194/acp-14-13223-2014, 2014
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This study presents in situ cloud microphysical observations obtained during a double flight in a Hector thunderstorm during the SCOUT-O3 campaign from Darwin, Northern Australia, in 2005. The measurements show a change of the micophysics with the storm's evolution. The clouds in the dissipating stage possess a high potential for affecting the humidity in the tropical tropopause layer.
K. P. Wyche, A. C. Ryan, C. N. Hewitt, M. R. Alfarra, G. McFiggans, T. Carr, P. S. Monks, K. L. Smallbone, G. Capes, J. F. Hamilton, T. A. M. Pugh, and A. R. MacKenzie
Atmos. Chem. Phys., 14, 12781–12801, https://doi.org/10.5194/acp-14-12781-2014, https://doi.org/10.5194/acp-14-12781-2014, 2014
J. D. Whitehead, M. Irwin, J. D. Allan, N. Good, and G. McFiggans
Atmos. Chem. Phys., 14, 11833–11841, https://doi.org/10.5194/acp-14-11833-2014, https://doi.org/10.5194/acp-14-11833-2014, 2014
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Water uptake of ambient particles was measured by 2 independent techniques at a wide range of locations between 2007 and 2013. The agreement between the techniques was mixed and hence the number of potential cloud seeds calculated from the measurements frequently showed discrepancies. Whilst there is sensitivity to how well we measure the size of the particles, much of the difference depends on how the particles behave when exposed to moisture in the different techniques (and in the atmosphere).
S. Archer-Nicholls, D. Lowe, S. Utembe, J. Allan, R. A. Zaveri, J. D. Fast, Ø. Hodnebrog, H. Denier van der Gon, and G. McFiggans
Geosci. Model Dev., 7, 2557–2579, https://doi.org/10.5194/gmd-7-2557-2014, https://doi.org/10.5194/gmd-7-2557-2014, 2014
M. J. Lawler, J. Whitehead, C. O'Dowd, C. Monahan, G. McFiggans, and J. N. Smith
Atmos. Chem. Phys., 14, 11557–11569, https://doi.org/10.5194/acp-14-11557-2014, https://doi.org/10.5194/acp-14-11557-2014, 2014
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This work describes the chemical and physical characterization of very small (< 100 nm diameter) particles in the marine atmosphere. We show that sea salt is present even at very small sizes and present evidence that organic species are important contributors to apparent new particle formation events over the ocean.
W. Woiwode, J.-U. Grooß, H. Oelhaf, S. Molleker, S. Borrmann, A. Ebersoldt, W. Frey, T. Gulde, S. Khaykin, G. Maucher, C. Piesch, and J. Orphal
Atmos. Chem. Phys., 14, 11525–11544, https://doi.org/10.5194/acp-14-11525-2014, https://doi.org/10.5194/acp-14-11525-2014, 2014
S. Molleker, S. Borrmann, H. Schlager, B. Luo, W. Frey, M. Klingebiel, R. Weigel, M. Ebert, V. Mitev, R. Matthey, W. Woiwode, H. Oelhaf, A. Dörnbrack, G. Stratmann, J.-U. Grooß, G. Günther, B. Vogel, R. Müller, M. Krämer, J. Meyer, and F. Cairo
Atmos. Chem. Phys., 14, 10785–10801, https://doi.org/10.5194/acp-14-10785-2014, https://doi.org/10.5194/acp-14-10785-2014, 2014
E. Simpson, P. Connolly, and G. McFiggans
Geosci. Model Dev., 7, 1535–1542, https://doi.org/10.5194/gmd-7-1535-2014, https://doi.org/10.5194/gmd-7-1535-2014, 2014
P. J. Connolly, D. O. Topping, F. Malavelle, and G. McFiggans
Atmos. Chem. Phys., 14, 2289–2302, https://doi.org/10.5194/acp-14-2289-2014, https://doi.org/10.5194/acp-14-2289-2014, 2014
H. Kokkola, P. Yli-Pirilä, M. Vesterinen, H. Korhonen, H. Keskinen, S. Romakkaniemi, L. Hao, A. Kortelainen, J. Joutsensaari, D. R. Worsnop, A. Virtanen, and K. E. J. Lehtinen
Atmos. Chem. Phys., 14, 1689–1700, https://doi.org/10.5194/acp-14-1689-2014, https://doi.org/10.5194/acp-14-1689-2014, 2014
M. R. Alfarra, N. Good, K. P. Wyche, J. F. Hamilton, P. S. Monks, A. C. Lewis, and G. McFiggans
Atmos. Chem. Phys., 13, 11769–11789, https://doi.org/10.5194/acp-13-11769-2013, https://doi.org/10.5194/acp-13-11769-2013, 2013
J. F. Hamilton, M. R. Alfarra, N. Robinson, M. W. Ward, A. C. Lewis, G. B. McFiggans, H. Coe, and J. D. Allan
Atmos. Chem. Phys., 13, 11295–11305, https://doi.org/10.5194/acp-13-11295-2013, https://doi.org/10.5194/acp-13-11295-2013, 2013
M. von Hobe, S. Bekki, S. Borrmann, F. Cairo, F. D'Amato, G. Di Donfrancesco, A. Dörnbrack, A. Ebersoldt, M. Ebert, C. Emde, I. Engel, M. Ern, W. Frey, S. Genco, S. Griessbach, J.-U. Grooß, T. Gulde, G. Günther, E. Hösen, L. Hoffmann, V. Homonnai, C. R. Hoyle, I. S. A. Isaksen, D. R. Jackson, I. M. Jánosi, R. L. Jones, K. Kandler, C. Kalicinsky, A. Keil, S. M. Khaykin, F. Khosrawi, R. Kivi, J. Kuttippurath, J. C. Laube, F. Lefèvre, R. Lehmann, S. Ludmann, B. P. Luo, M. Marchand, J. Meyer, V. Mitev, S. Molleker, R. Müller, H. Oelhaf, F. Olschewski, Y. Orsolini, T. Peter, K. Pfeilsticker, C. Piesch, M. C. Pitts, L. R. Poole, F. D. Pope, F. Ravegnani, M. Rex, M. Riese, T. Röckmann, B. Rognerud, A. Roiger, C. Rolf, M. L. Santee, M. Scheibe, C. Schiller, H. Schlager, M. Siciliani de Cumis, N. Sitnikov, O. A. Søvde, R. Spang, N. Spelten, F. Stordal, O. Sumińska-Ebersoldt, A. Ulanovski, J. Ungermann, S. Viciani, C. M. Volk, M. vom Scheidt, P. von der Gathen, K. Walker, T. Wegner, R. Weigel, S. Weinbruch, G. Wetzel, F. G. Wienhold, I. Wohltmann, W. Woiwode, I. A. K. Young, V. Yushkov, B. Zobrist, and F. Stroh
Atmos. Chem. Phys., 13, 9233–9268, https://doi.org/10.5194/acp-13-9233-2013, https://doi.org/10.5194/acp-13-9233-2013, 2013
P. J. Connolly, G. Vaughan, P. Cook, G. Allen, H. Coe, T. W. Choularton, C. Dearden, and A. Hill
Atmos. Chem. Phys., 13, 7133–7152, https://doi.org/10.5194/acp-13-7133-2013, https://doi.org/10.5194/acp-13-7133-2013, 2013
J. Skrotzki, P. Connolly, M. Schnaiter, H. Saathoff, O. Möhler, R. Wagner, M. Niemand, V. Ebert, and T. Leisner
Atmos. Chem. Phys., 13, 4451–4466, https://doi.org/10.5194/acp-13-4451-2013, https://doi.org/10.5194/acp-13-4451-2013, 2013
D. Liu, J. Allan, J. Whitehead, D. Young, M. Flynn, H. Coe, G. McFiggans, Z. L. Fleming, and B. Bandy
Atmos. Chem. Phys., 13, 2015–2029, https://doi.org/10.5194/acp-13-2015-2013, https://doi.org/10.5194/acp-13-2015-2013, 2013
Related subject area
Subject: Clouds and Precipitation | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Physics (physical properties and processes)
Stable and unstable fall motions of plate-like ice crystal analogues
Secondary ice production – no evidence of efficient rime-splintering mechanism
Fragmentation of ice particles: laboratory experiments on graupel–graupel and graupel–snowflake collisions
Molecular simulations reveal that heterogeneous ice nucleation occurs at higher temperatures in water under capillary tension
Measurement of the collision rate coefficients between atmospheric ions and multiply charged aerosol particles in the CERN CLOUD chamber
Re-evaluating cloud chamber constraints on depositional ice growth in cirrus clouds – Part 1: Model description and sensitivity tests
Ice nucleation by smectites: the role of the edges
A single-parameter hygroscopicity model for functionalized insoluble aerosol surfaces
Mexican agricultural soil dust as a source of ice nucleating particles
The impact of (bio-)organic substances on the ice nucleation activity of the K-feldspar microcline in aqueous solutions
Secondary ice production during the break-up of freezing water drops on impact with ice particles
High homogeneous freezing onsets of sulfuric acid aerosol at cirrus temperatures
Laboratory and field studies of ice-nucleating particles from open-lot livestock facilities in Texas
Comment on “Review of experimental studies of secondary ice production” by Korolev and Leisner (2020)
Effect of chemically induced fracturing on the ice nucleation activity of alkali feldspar
Ice nucleation ability of ammonium sulfate aerosol particles internally mixed with secondary organics
Ice-nucleating particles in precipitation samples from the Texas Panhandle
Comparative study on immersion freezing utilizing single-droplet levitation methods
Exploratory experiments on pre-activated freezing nucleation on mercuric iodide
Application of holography and automated image processing for laboratory experiments on mass and fall speed of small cloud ice crystals
Review of experimental studies of secondary ice production
The role of contact angle and pore width on pore condensation and freezing
Technical note: Equilibrium droplet size distributions in a turbulent cloud chamber with uniform supersaturation
Protein aggregates nucleate ice: the example of apoferritin
No anomalous supersaturation in ultracold cirrus laboratory experiments
Lateral facet growth of ice and snow – Part 1: Observations and applications to secondary habits
The ice-nucleating ability of quartz immersed in water and its atmospheric importance compared to K-feldspar
Ice nucleation properties of K-feldspar polymorphs and plagioclase feldspars
Enhanced ice nucleation activity of coal fly ash aerosol particles initiated by ice-filled pores
A comprehensive characterization of ice nucleation by three different types of cellulose particles immersed in water
Activation of intact bacteria and bacterial fragments mixed with agar as cloud droplets and ice crystals in cloud chamber experiments
Anomalous holiday precipitation over southern China
Coal fly ash: linking immersion freezing behavior and physicochemical particle properties
Surface roughness during depositional growth and sublimation of ice crystals
Ice nucleation abilities of soot particles determined with the Horizontal Ice Nucleation Chamber
Uncertainty in counting ice nucleating particles with continuous flow diffusion chambers
Experimental evidence of the rear capture of aerosol particles by raindrops
Refreeze experiments with water droplets containing different types of ice nuclei interpreted by classical nucleation theory
Pre-activation of aerosol particles by ice preserved in pores
Heterogeneous ice nucleation on dust particles sourced from nine deserts worldwide – Part 1: Immersion freezing
A comparative study of K-rich and Na/Ca-rich feldspar ice-nucleating particles in a nanoliter droplet freezing assay
Ice nucleation efficiency of AgI: review and new insights
The adsorption of fungal ice-nucleating proteins on mineral dusts: a terrestrial reservoir of atmospheric ice-nucleating particles
Exploring an approximation for the homogeneous freezing temperature of water droplets
Cloud chamber experiments on the origin of ice crystal complexity in cirrus clouds
Phase transition observations and discrimination of small cloud particles by light polarization in expansion chamber experiments
Analysis of isothermal and cooling-rate-dependent immersion freezing by a unifying stochastic ice nucleation model
Pre-activation of ice-nucleating particles by the pore condensation and freezing mechanism
Influence of the ambient humidity on the concentration of natural deposition-mode ice-nucleating particles
Comparison of measured and calculated collision efficiencies at low temperatures
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.
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
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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
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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.
Peter A. Alpert and Daniel A. Knopf
Atmos. Chem. Phys., 16, 2083–2107, https://doi.org/10.5194/acp-16-2083-2016, https://doi.org/10.5194/acp-16-2083-2016, 2016
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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.
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
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.
The coupled system of the Manchester Aerosol Chamber and Manchester Ice Cloud Chamber was used...
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