Articles | Volume 14, issue 16
Atmos. Chem. Phys., 14, 8501–8520, 2014
https://doi.org/10.5194/acp-14-8501-2014
© Author(s) 2014. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Atmos. Chem. Phys., 14, 8501–8520, 2014
https://doi.org/10.5194/acp-14-8501-2014
© Author(s) 2014. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article 22 Aug 2014
Research article | 22 Aug 2014
Representing time-dependent freezing behaviour in immersion mode ice nucleation
R. J. Herbert et al.
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Marine stratocumulus clouds cover large regions of the ocean and act to cool the climate. We use high-resolution simulations to understand how observed layers of elevated smoke impact stratocumulus via the solar heating that occurs within the smoke layer. We find that the cloud response is strongest for thin, dense layers of smoke close to the cloud. The response rapidly weakens as the cloud-to-smoke gap increases. Generally, the smoke acts to thicken clouds and enhance their cooling effect.
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Mineral dust and particles of biological origin are important types of ice-nucleating particles (INP) that can trigger ice formation of supercooled cloud droplets. Heat treatments are used to “detect” the presence of biological INP in samples collected from the environment as the activity of mineral INP is assumed unchanged, yet this has not been fully assessed. We show that the ice-nucleating ability of some minerals can change after heating and discuss how INP heat tests should be interpreted.
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Heather Guy, Ian M. Brooks, Ken S. Carslaw, Benjamin J. Murray, Von P. Walden, Matthew D. Shupe, Claire Pettersen, David D. Turner, Christopher J. Cox, William D. Neff, Ralf Bennartz, and Ryan R. Neely III
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We present the first full year of surface aerosol number concentration measurements from the central Greenland Ice Sheet. Aerosol concentrations here have an opposite seasonal cycle to those at lower altitude Arctic sites, which is driven by large-scale atmospheric circulation. Our results can be used to help understand the role aerosols might play in Greenland surface melt through the modification of cloud properties. This is crucial in a rapidly changing region where observations are sparse.
Rachel E. Hawker, Annette K. Miltenberger, Jonathan M. Wilkinson, Adrian A. Hill, Ben J. Shipway, Zhiqiang Cui, Richard J. Cotton, Ken S. Carslaw, Paul R. Field, and Benjamin J. Murray
Atmos. Chem. Phys., 21, 5439–5461, https://doi.org/10.5194/acp-21-5439-2021, https://doi.org/10.5194/acp-21-5439-2021, 2021
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Julia Schneider, Kristina Höhler, Paavo Heikkilä, Jorma Keskinen, Barbara Bertozzi, Pia Bogert, Tobias Schorr, Nsikanabasi Silas Umo, Franziska Vogel, Zoé Brasseur, Yusheng Wu, Simo Hakala, Jonathan Duplissy, Dmitri Moisseev, Markku Kulmala, Michael P. Adams, Benjamin J. Murray, Kimmo Korhonen, Liqing Hao, Erik S. Thomson, Dimitri Castarède, Thomas Leisner, Tuukka Petäjä, and Ottmar Möhler
Atmos. Chem. Phys., 21, 3899–3918, https://doi.org/10.5194/acp-21-3899-2021, https://doi.org/10.5194/acp-21-3899-2021, 2021
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By triggering the formation of ice crystals, ice-nucleating particles (INP) strongly influence cloud formation. Continuous, long-term measurements are needed to characterize the atmospheric INP variability. Here, a first long-term time series of INP spectra measured in the boreal forest for more than 1 year is presented, showing a clear seasonal cycle. It is shown that the seasonal dependency of INP concentrations and prevalent INP types is driven by the abundance of biogenic aerosol.
Ottmar Möhler, Michael Adams, Larissa Lacher, Franziska Vogel, Jens Nadolny, Romy Ullrich, Cristian Boffo, Tatjana Pfeuffer, Achim Hobl, Maximilian Weiß, Hemanth S. K. Vepuri, Naruki Hiranuma, and Benjamin J. Murray
Atmos. Meas. Tech., 14, 1143–1166, https://doi.org/10.5194/amt-14-1143-2021, https://doi.org/10.5194/amt-14-1143-2021, 2021
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Luisa Ickes, Grace C. E. Porter, Robert Wagner, Michael P. Adams, Sascha Bierbauer, Allan K. Bertram, Merete Bilde, Sigurd Christiansen, Annica M. L. Ekman, Elena Gorokhova, Kristina Höhler, Alexei A. Kiselev, Caroline Leck, Ottmar Möhler, Benjamin J. Murray, Thea Schiebel, Romy Ullrich, and Matthew E. Salter
Atmos. Chem. Phys., 20, 11089–11117, https://doi.org/10.5194/acp-20-11089-2020, https://doi.org/10.5194/acp-20-11089-2020, 2020
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The Arctic is a region where aerosols are scarce. Sea spray might be a potential source of aerosols acting as ice-nucleating particles. We investigate two common phytoplankton species (Melosira arctica and Skeletonema marinoi) and present their ice nucleation activity in comparison with Arctic seawater microlayer samples from different field campaigns. We also aim to understand the aerosolization process of marine biological samples and the potential effect on the ice nucleation activity.
Grace C. E. Porter, Sebastien N. F. Sikora, Michael P. Adams, Ulrike Proske, Alexander D. Harrison, Mark D. Tarn, Ian M. Brooks, and Benjamin J. Murray
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Ice-nucleating particles affect cloud development, lifetime, and radiative properties. Hence it is important to know the abundance of INPs throughout the atmosphere. Here we present the development and application of a radio-controlled payload capable of collecting size-resolved aerosol from a tethered balloon for the primary purpose of offline INP analysis. Test data are presented from four locations: southern Finland, northern England, Svalbard, and southern England.
Ross J. Herbert, Nicolas Bellouin, Ellie J. Highwood, and Adrian A. Hill
Atmos. Chem. Phys., 20, 1317–1340, https://doi.org/10.5194/acp-20-1317-2020, https://doi.org/10.5194/acp-20-1317-2020, 2020
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Marine stratocumulus clouds cover large regions of the ocean and act to cool the climate. We use high-resolution simulations to understand how observed layers of elevated smoke impact stratocumulus via the solar heating that occurs within the smoke layer. We find that the cloud response is strongest for thin, dense layers of smoke close to the cloud. The response rapidly weakens as the cloud-to-smoke gap increases. Generally, the smoke acts to thicken clouds and enhance their cooling effect.
Alberto Sanchez-Marroquin, Duncan H. P. Hedges, Matthew Hiscock, Simon T. Parker, Philip D. Rosenberg, Jamie Trembath, Richard Walshaw, Ian T. Burke, James B. McQuaid, and Benjamin J. Murray
Atmos. Meas. Tech., 12, 5741–5763, https://doi.org/10.5194/amt-12-5741-2019, https://doi.org/10.5194/amt-12-5741-2019, 2019
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Sampling coarse-mode aerosol from a fast-moving research aircraft is challenging and can be subject to substantial losses and enhancements. We characterise these losses and enhancements for an inlet system designed to collect aerosol onto filters. We go on to present an application of this inlet system where we use electron microscopy to study the size and composition of the collected aerosol particles.
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.
Elena C. Maters, Donald B. Dingwell, Corrado Cimarelli, Dirk Müller, Thomas F. Whale, and Benjamin J. Murray
Atmos. Chem. Phys., 19, 5451–5465, https://doi.org/10.5194/acp-19-5451-2019, https://doi.org/10.5194/acp-19-5451-2019, 2019
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This experimental study investigates the influence of volcanic ash chemical composition, crystallinity, and mineralogy on its ability to promote freezing of supercooled water. The results indicate that crystals in ash play a key role in this process and suggest that feldspars and perhaps pyroxenes in ash may be highly ice-active. These findings contribute to improving understanding of the potential of ash emissions from different explosive eruptions to impact ice formation in the atmosphere.
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.
Claire L. Ryder, Franco Marenco, Jennifer K. Brooke, Victor Estelles, Richard Cotton, Paola Formenti, James B. McQuaid, Hannah C. Price, Dantong Liu, Patrick Ausset, Phil D. Rosenberg, Jonathan W. Taylor, Tom Choularton, Keith Bower, Hugh Coe, Martin Gallagher, Jonathan Crosier, Gary Lloyd, Eleanor J. Highwood, and Benjamin J. Murray
Atmos. Chem. Phys., 18, 17225–17257, https://doi.org/10.5194/acp-18-17225-2018, https://doi.org/10.5194/acp-18-17225-2018, 2018
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Every year, millions of tons of Saharan dust particles are carried across the Atlantic by the wind, where they can affect weather patterns and climate. Their sizes span orders of magnitude, but the largest (over 10 microns – around the width of a human hair) are difficult to measure and few observations exist. Here we show new aircraft observations of large dust particles, finding more than we would expect, and we quantify their properties which allow them to interact with atmospheric radiation.
Paul J. DeMott, Ottmar Möhler, Daniel J. Cziczo, Naruki Hiranuma, Markus D. Petters, Sarah S. Petters, Franco Belosi, Heinz G. Bingemer, Sarah D. Brooks, Carsten Budke, Monika Burkert-Kohn, Kristen N. Collier, Anja Danielczok, Oliver Eppers, Laura Felgitsch, Sarvesh Garimella, Hinrich Grothe, Paul Herenz, Thomas C. J. Hill, Kristina Höhler, Zamin A. Kanji, Alexei Kiselev, Thomas Koop, Thomas B. Kristensen, Konstantin Krüger, Gourihar Kulkarni, Ezra J. T. Levin, Benjamin J. Murray, Alessia Nicosia, Daniel O'Sullivan, Andreas Peckhaus, Michael J. Polen, Hannah C. Price, Naama Reicher, Daniel A. Rothenberg, Yinon Rudich, Gianni Santachiara, Thea Schiebel, Jann Schrod, Teresa M. Seifried, Frank Stratmann, Ryan C. Sullivan, Kaitlyn J. Suski, Miklós Szakáll, Hans P. Taylor, Romy Ullrich, Jesus Vergara-Temprado, Robert Wagner, Thomas F. Whale, Daniel Weber, André Welti, Theodore W. Wilson, Martin J. Wolf, and Jake Zenker
Atmos. Meas. Tech., 11, 6231–6257, https://doi.org/10.5194/amt-11-6231-2018, https://doi.org/10.5194/amt-11-6231-2018, 2018
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The ability to measure ice nucleating particles is vital to quantifying their role in affecting clouds and precipitation. Methods for measuring droplet freezing were compared while co-sampling relevant particle types. Measurement correspondence was very good for ice nucleating particles of bacterial and natural soil origin, and somewhat more disparate for those of mineral origin. Results reflect recently improved capabilities and provide direction toward addressing remaining measurement issues.
Meng Si, Victoria E. Irish, Ryan H. Mason, Jesús Vergara-Temprado, Sarah J. Hanna, Luis A. Ladino, Jacqueline D. Yakobi-Hancock, Corinne L. Schiller, Jeremy J. B. Wentzell, Jonathan P. D. Abbatt, Ken S. Carslaw, Benjamin J. Murray, and Allan K. Bertram
Atmos. Chem. Phys., 18, 15669–15685, https://doi.org/10.5194/acp-18-15669-2018, https://doi.org/10.5194/acp-18-15669-2018, 2018
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Using the concentrations of ice-nucleating particles (INPs) and total aerosol particles measured at three coastal marine sites, the ice-nucleating ability of aerosol particles on a per number basis and a per surface-area basis were determined as a function of size. The ice-nucleating ability was strongly dependent on size, with larger particles being more efficient. This type of information can help determine the sources of INPs and constrain the future modelling of INPs and mixed-phase clouds.
Alexander D. Harrison, Thomas F. Whale, Rupert Rutledge, Stephen Lamb, Mark D. Tarn, Grace C. E. Porter, Michael P. Adams, James B. McQuaid, George J. Morris, and Benjamin J. Murray
Atmos. Meas. Tech., 11, 5629–5641, https://doi.org/10.5194/amt-11-5629-2018, https://doi.org/10.5194/amt-11-5629-2018, 2018
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The detection of low concentrations of ice-nucleating particles (INPs) is challenging. Here we present a new technique (IR-NIPI) that is sensitive to low concentrations of INPs (> 0.01 L−1) and uses an infrared camera with a novel calibration to detect the freezing of experimental suspensions. IR-NIPI temperature measurements prove to be robust with a series of comparisons to thermocouple measurements. Experimental comparisons to other freezing assay instruments are also in agreement.
Alexander D. James, James S. A. Brooke, Thomas P. Mangan, Thomas F. Whale, John M. C. Plane, and Benjamin J. Murray
Atmos. Chem. Phys., 18, 4519–4531, https://doi.org/10.5194/acp-18-4519-2018, https://doi.org/10.5194/acp-18-4519-2018, 2018
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Crystal nucleation in polar stratospheric clouds (PSCs) has a direct impact on stratospheric chemistry and ozone. However, the mechanism of nucleation has been unclear for decades, limiting prediction of the response of ozone to atmospheric changes. We experimentally demonstrate that meteoric material can trigger nucleation heterogeneously and this can produce observed crystal concentrations in PSCs. This discovery paves the way to robust modelling of past and future trends in PSCs and ozone.
Victoria E. Irish, Pablo Elizondo, Jessie Chen, Cédric Chou, Joannie Charette, Martine Lizotte, Luis A. Ladino, Theodore W. Wilson, Michel Gosselin, Benjamin J. Murray, Elena Polishchuk, Jonathan P. D. Abbatt, Lisa A. Miller, and Allan K. Bertram
Atmos. Chem. Phys., 17, 10583–10595, https://doi.org/10.5194/acp-17-10583-2017, https://doi.org/10.5194/acp-17-10583-2017, 2017
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The ocean is a possible source of atmospheric ice-nucleating particles (INPs). In this study we found that INPs were ubiquitous in the sea-surface microlayer and bulk seawater in the Canadian Arctic. A strong negative correlation was observed between salinity and freezing temperatures (after correcting for freezing point depression). Heat and filtration treatments of the samples showed that the INPs were likely biological material with sizes between 0.02 μm and 0.2 μm in diameter.
Jesús Vergara-Temprado, Benjamin J. Murray, Theodore W. Wilson, Daniel O'Sullivan, Jo Browse, Kirsty J. Pringle, Karin Ardon-Dryer, Allan K. Bertram, Susannah M. Burrows, Darius Ceburnis, Paul J. DeMott, Ryan H. Mason, Colin D. O'Dowd, Matteo Rinaldi, and Ken S. Carslaw
Atmos. Chem. Phys., 17, 3637–3658, https://doi.org/10.5194/acp-17-3637-2017, https://doi.org/10.5194/acp-17-3637-2017, 2017
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We quantify the importance in the atmosphere of different aerosol components to contribute to global ice-nucleating particles concentrations (INPs). The aim is to improve the way atmospheric cloud-ice processes are represented in climate models so they will be able to make better predictions in the future. We found that a kind of dust (K-feldspar), together with marine organic aerosols, can help to improve the representation of INPs and explain most of their observations.
Alexander D. Harrison, Thomas F. Whale, Michael A. Carpenter, Mark A. Holden, Lesley Neve, Daniel O'Sullivan, Jesus Vergara Temprado, and Benjamin J. Murray
Atmos. Chem. Phys., 16, 10927–10940, https://doi.org/10.5194/acp-16-10927-2016, https://doi.org/10.5194/acp-16-10927-2016, 2016
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Mineral dust particles are known to act as effective ice nucleating particles in the atmosphere and to play a role in the glaciation of mixed phase clouds. We have measured the ice nucleation activity of 15 different feldspar samples using a droplet freezing experiment and shown that alkali feldspars nucleate ice much more efficiently than plagioclase feldspars. We have also shown that certain "hyper-active" alkali feldspars nucleate ice very efficiently compared to typical alkali feldspars.
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.
G. Vali, P. J. DeMott, O. Möhler, and T. F. Whale
Atmos. Chem. Phys., 15, 10263–10270, https://doi.org/10.5194/acp-15-10263-2015, https://doi.org/10.5194/acp-15-10263-2015, 2015
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Clarification is needed in the terminology used to discuss ice nucleation in the literature. Conflicting interpretations coupled with uncertainties about the details of the processes have led to difficulties in the clear communication of results and ideas. This paper contains a proposal for future usage. This proposed terminology was arrived at as a result of a year-long exchange of suggestions by a number of scientists.
T. F. Whale, B. J. Murray, D. O'Sullivan, T. W. Wilson, N. S. Umo, K. J. Baustian, J. D. Atkinson, D. A. Workneh, and G. J. Morris
Atmos. Meas. Tech., 8, 2437–2447, https://doi.org/10.5194/amt-8-2437-2015, https://doi.org/10.5194/amt-8-2437-2015, 2015
N. S. Umo, B. J. Murray, M. T. Baeza-Romero, J. M. Jones, A. R. Lea-Langton, T. L. Malkin, D. O'Sullivan, L. Neve, J. M. C. Plane, and A. Williams
Atmos. Chem. Phys., 15, 5195–5210, https://doi.org/10.5194/acp-15-5195-2015, https://doi.org/10.5194/acp-15-5195-2015, 2015
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Combustion ash particles nucleate ice in the immersion mode at conditions relevant to mixed-phase clouds. Hence, combustion ashes could play an important role in primary ice formation in mixed-phase clouds, especially in clouds that are formed near the emission source of these aerosol particles. From this study, there is a need to quantify the atmospheric abundance of combustion ashes in order to quantitatively assess the impact of combustion ashes on mixed-phase clouds.
N. Hiranuma, S. Augustin-Bauditz, H. Bingemer, C. Budke, J. Curtius, A. Danielczok, K. Diehl, K. Dreischmeier, M. Ebert, F. Frank, N. Hoffmann, K. Kandler, A. Kiselev, T. Koop, T. Leisner, O. Möhler, B. Nillius, A. Peckhaus, D. Rose, S. Weinbruch, H. Wex, Y. Boose, P. J. DeMott, J. D. Hader, T. C. J. Hill, Z. A. Kanji, G. Kulkarni, E. J. T. Levin, C. S. McCluskey, M. Murakami, B. J. Murray, D. Niedermeier, M. D. Petters, D. O'Sullivan, A. Saito, G. P. Schill, T. Tajiri, M. A. Tolbert, A. Welti, T. F. Whale, T. P. Wright, and K. Yamashita
Atmos. Chem. Phys., 15, 2489–2518, https://doi.org/10.5194/acp-15-2489-2015, https://doi.org/10.5194/acp-15-2489-2015, 2015
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Seventeen ice nucleation measurement techniques contributed to investigate the immersion freezing behavior of illite NX. All data showed a similar temperature trend, but the measured ice nucleation activity was on average smaller for the wet suspended samples and higher for the dry-dispersed aerosol samples at high temperatures. A continued investigation and collaboration is necessary to obtain further insights into consistency or diversity of ice nucleation measurements.
H. C. Price, B. J. Murray, J. Mattsson, D. O'Sullivan, T. W. Wilson, K. J. Baustian, and L. G. Benning
Atmos. Chem. Phys., 14, 3817–3830, https://doi.org/10.5194/acp-14-3817-2014, https://doi.org/10.5194/acp-14-3817-2014, 2014
D. O'Sullivan, B. J. Murray, T. L. Malkin, T. F. Whale, N. S. Umo, J. D. Atkinson, H. C. Price, K. J. Baustian, J. Browse, and M. E. Webb
Atmos. Chem. Phys., 14, 1853–1867, https://doi.org/10.5194/acp-14-1853-2014, https://doi.org/10.5194/acp-14-1853-2014, 2014
Related subject area
Subject: Aerosols | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Physics (physical properties and processes)
Heterogeneous ice nucleation ability of aerosol particles generated from Arctic sea surface microlayer and surface seawater samples at cirrus temperatures
Aerosol formation and growth rates from chamber experiments using Kalman smoothing
Phase state of secondary organic aerosol in chamber photo-oxidation of mixed precursors
Ice nucleation on surrogates of boreal forest SOA particles: effect of water content and oxidative age
Viscosity and phase state of aerosol particles consisting of sucrose mixed with inorganic salts
Observations on hygroscopic growth and phase transitions of mixed 1, 2, 6-hexanetriol ∕ (NH4)2SO4 particles: investigation of the liquid–liquid phase separation (LLPS) dynamic process and mechanism and secondary LLPS during the dehumidification
Boundary layer structure characteristics under objective classification of persistent pollution weather types in the Beijing area
Technical Note: Pyrolysis principles explain time-resolved organic aerosol release from biomass burning
Properties and emission factors of cloud condensation nuclei from biomass cookstoves – observations of a strong dependency on potassium content in the fuel
Measurement report: Effects of NOx and seed aerosol on highly oxygenated organic molecules (HOMs) from cyclohexene ozonolysis
Interactions of organosulfates with water vapor under sub- and supersaturated conditions
Laboratory study of the collection efficiency of submicron aerosol particles by cloud droplets – Part I: Influence of relative humidity
The effect of (NH4)2SO4 on the freezing properties of non-mineral dust ice nucleating substances of atmospheric relevance
Size-resolved atmospheric ice-nucleating particles during East Asian dust events
Aqueous-phase behavior of glyoxal and methylglyoxal observed with carbon and oxygen K-edge X-ray absorption spectroscopy
Brown carbon's emission factors and optical characteristics in household biomass burning: developing a novel algorithm for estimating the contribution of brown carbon
Effect of mixing structure on the water uptake of mixtures of ammonium sulfate and phthalic acid particles
Toward closure between predicted and observed particle viscosity over a wide range of temperatures and relative humidity
The effects of morphology, mobility size, and secondary organic aerosol (SOA) material coating on the ice nucleation activity of black carbon in the cirrus regime
The ice-nucleating activity of Arctic sea surface microlayer samples and marine algal cultures
Comparing secondary organic aerosol (SOA) volatility distributions derived from isothermal SOA particle evaporation data and FIGAERO–CIMS measurements
Laboratory studies of fresh and aged biomass burning aerosol emitted from east African biomass fuels – Part 1: Optical properties
Enhanced growth rate of atmospheric particles from sulfuric acid
Composition and volatility of secondary organic aerosol (SOA) formed from oxidation of real tree emissions compared to simplified volatile organic compound (VOC) systems
Effects of SO2 on optical properties of secondary organic aerosol generated from photooxidation of toluene under different relative humidity conditions
Influence of the dry aerosol particle size distribution and morphology on the cloud condensation nuclei activation. An experimental and theoretical investigation
Experimental investigation into the volatilities of highly oxygenated organic molecules (HOMs)
Detection of tar brown carbon with a single particle soot photometer (SP2)
Complex refractive indices and single-scattering albedo of global dust aerosols in the shortwave spectrum and relationship to size and iron content
Technical note: Frenkel, Halsey and Hill analysis of water on clay minerals: toward closure between cloud condensation nuclei activity and water adsorption
Liquid–liquid phase separation and viscosity within secondary organic aerosol generated from diesel fuel vapors
Laboratory study of the heterogeneous ice nucleation on black-carbon-containing aerosol
Specifying the light-absorbing properties of aerosol particles in fresh snow samples, collected at the Environmental Research Station Schneefernerhaus (UFS), Zugspitze
Optimization of process models for determining volatility distribution and viscosity of organic aerosols from isothermal particle evaporation data
Inversely modeling homogeneous H2SO4 − H2O nucleation rate in exhaust-related conditions
The importance of crystalline phases in ice nucleation by volcanic ash
Heterogeneous ice nucleation properties of natural desert dust particles coated with a surrogate of secondary organic aerosol
Cloud condensation nuclei activity of six pollenkitts and the influence of their surface activity
Links of climate variability in Arctic sea ice, Eurasian teleconnection pattern and summer surface ozone pollution in North China
The effect of hydrophobic glassy organic material on the cloud condensation nuclei activity of particles with different morphologies
Technical note: The role of evolving surface tension in the formation of cloud droplets
Physical properties of secondary photochemical aerosol from OH oxidation of a cyclic siloxane
Cloud droplet activation of secondary organic aerosol is mainly controlled by molecular weight, not water solubility
Production of particulate brown carbon during atmospheric aging of residential wood-burning emissions
Evaluating the performance of two surface layer schemes for the momentum and heat exchange processes during severe haze pollution in Jing-Jin-Ji in eastern China
Measured particle water uptake enhanced by co-condensing vapours
Cloud droplet activation of black carbon particles coated with organic compounds of varying solubility
Measurement and modeling of the multiwavelength optical properties of uncoated flame-generated soot
Liquid–liquid phase separation in organic particles containing one and two organic species: importance of the average O : C
Establishing the impact of model surfactants on cloud condensation nuclei activity of sea spray aerosol mimics
Robert Wagner, Luisa Ickes, Allan K. Bertram, Nora Els, Elena Gorokhova, Ottmar Möhler, Benjamin J. Murray, Nsikanabasi Silas Umo, and Matthew E. Salter
Atmos. Chem. Phys., 21, 13903–13930, https://doi.org/10.5194/acp-21-13903-2021, https://doi.org/10.5194/acp-21-13903-2021, 2021
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Sea spray aerosol particles are a mixture of inorganic salts and organic matter from phytoplankton organisms. At low temperatures in the upper troposphere, both inorganic and organic constituents can induce the formation of ice crystals and thereby impact cloud properties and climate. In this study, we performed experiments in a cloud simulation chamber with particles produced from Arctic seawater samples to quantify the relative contribution of inorganic and organic species in ice formation.
Matthew Ozon, Dominik Stolzenburg, Lubna Dada, Aku Seppänen, and Kari E. J. Lehtinen
Atmos. Chem. Phys., 21, 12595–12611, https://doi.org/10.5194/acp-21-12595-2021, https://doi.org/10.5194/acp-21-12595-2021, 2021
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Measuring the rate at which aerosol particles are formed is of importance for understanding climate change. We present an analysis method based on Kalman smoothing, which retrieves new particle formation and growth rates from size-distribution measurements. We apply it to atmospheric simulation chamber experiments and show that it agrees well with traditional methods. In addition, it provides reliable uncertainty estimates, and we suggest instrument design optimisation for signal processing.
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.
Young-Chul Song, Joseph Lilek, Jae Bong Lee, Man Nin Chan, Zhijun Wu, Andreas Zuend, and Mijung Song
Atmos. Chem. Phys., 21, 10215–10228, https://doi.org/10.5194/acp-21-10215-2021, https://doi.org/10.5194/acp-21-10215-2021, 2021
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We report viscosity of binary mixtures of organic material / H2O and inorganic salts / H2O, as well as ternary mixtures of organic material / inorganic salts/ H2O, over the atmospheric relative humidity (RH) range. The viscosity measurements indicate that the studied mixed organic–inorganic particles range in phase state from liquid to semi-solid or even solid across the atmospheric RH range at a temperature of 293 K.
Shuaishuai Ma, Zhe Chen, Shufeng Pang, and Yunhong Zhang
Atmos. Chem. Phys., 21, 9705–9717, https://doi.org/10.5194/acp-21-9705-2021, https://doi.org/10.5194/acp-21-9705-2021, 2021
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LLPS, efflorescence and deliquescence of aerosol particles can be observed visually and determined quantitatively. Different LLPS mechanisms may dominate successively in mixed organic–inorganic particles. The formation of more concentrated inorganic inclusions may cause secondary LLPS. Furthermore, high inorganic factions may result in an inorganic salt crust enclosing the separated organic phases.
Zhaobin Sun, Xiujuan Zhao, Ziming Li, Guiqian Tang, and Shiguang Miao
Atmos. Chem. Phys., 21, 8863–8882, https://doi.org/10.5194/acp-21-8863-2021, https://doi.org/10.5194/acp-21-8863-2021, 2021
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Different weather types will shape significantly different structures of the pollution boundary layer. The findings of this study allow us to understand the inherent difference among heavy pollution boundary layers; in addition, they reveal the formation mechanism of haze pollution from an integrated synoptic-scale and boundary layer structure perspective.
Mariam Fawaz, Anita Avery, Timothy B. Onasch, Leah R. Williams, and Tami C. Bond
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-380, https://doi.org/10.5194/acp-2021-380, 2021
Revised manuscript accepted for ACP
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Biomass burning is responsible for 90 % of the emissions of primary organic aerosols to the atmosphere. Emissions from biomass burning sources are considered chaotic. In this work, we developed a controlled experimental approach to understand the controlling factors in emission. Our results showed that emissions are repeatable and deterministic and that emissions from wood can be constrained.
Thomas Bjerring Kristensen, John Falk, Robert Lindgren, Christina Andersen, Vilhelm B. Malmborg, Axel C. Eriksson, Kimmo Korhonen, Ricardo Luis Carvalho, Christoffer Boman, Joakim Pagels, and Birgitta Svenningsson
Atmos. Chem. Phys., 21, 8023–8044, https://doi.org/10.5194/acp-21-8023-2021, https://doi.org/10.5194/acp-21-8023-2021, 2021
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Residential biomass combustion is a major anthropogenic source of aerosol particles on regional and global scales. Nevertheless, little is known about those aerosol particles' ability to act as cloud condensation nuclei (CCN) and thus influence cloud properties and climate. Our study shows a strong link between the potassium content in the fuel and emissions of CCN for different stove technologies. Previous studies may have underestimated the anthropogenic climate impact of these emissions.
Meri Räty, Otso Peräkylä, Matthieu Riva, Lauriane Quéléver, Olga Garmash, Matti Rissanen, and Mikael Ehn
Atmos. Chem. Phys., 21, 7357–7372, https://doi.org/10.5194/acp-21-7357-2021, https://doi.org/10.5194/acp-21-7357-2021, 2021
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Cyclohexene resembles certain relatively complex compounds in the atmosphere that through oxidation produce vapours that take part in aerosol formation. We studied the highly oxygenated organic molecules (HOMs) formed in cyclohexene ozonolysis, the relationship between their chemical composition and their tendency to condense onto seed aerosol, as well as the effect of NOx pollutants on their signals. Two existing models were also tested for their ability to predict the volatility of the HOMs.
Chao Peng, Patricia N. Razafindrambinina, Kotiba A. Malek, Lanxiadi Chen, Weigang Wang, Ru-Jin Huang, Yuqing Zhang, Xiang Ding, Maofa Ge, Xinming Wang, Akua A. Asa-Awuku, and Mingjin Tang
Atmos. Chem. Phys., 21, 7135–7148, https://doi.org/10.5194/acp-21-7135-2021, https://doi.org/10.5194/acp-21-7135-2021, 2021
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Organosulfates are important constituents in tropospheric aerosol particles, but their hygroscopic properties and cloud condensation nuclei activities are not well understood. In our work, three complementary techniques were employed to investigate the interactions of 11 organosulfates with water vapor under sub- and supersaturated conditions.
Alexis Dépée, Pascal Lemaitre, Thomas Gelain, Marie Monier, and Andrea Flossmann
Atmos. Chem. Phys., 21, 6945–6962, https://doi.org/10.5194/acp-21-6945-2021, https://doi.org/10.5194/acp-21-6945-2021, 2021
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Present article describe a new In-Cloud Aerosol Scavenging Experiment (In-CASE) that has been conceived to measure the collection efficiency of submicron aerosol particles by cloud droplets. The present article focuses on the influence of phoretic effects on the collection efficiency.
Soleil E. Worthy, Anand Kumar, Yu Xi, Jingwei Yun, Jessie Chen, Cuishan Xu, Victoria E. Irish, Pierre Amato, and Allan K. Bertram
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-245, https://doi.org/10.5194/acp-2021-245, 2021
Revised manuscript accepted for ACP
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We studied the effect of (NH4)2SO4 on the immersion freezing of non-mineral dust ice nucleating substances (INSs) and mineral dusts. (NH4)2SO4 had no effect on the median freezing temperature of nine of the ten tested non-mineral dust INSs, slightly decreased that of the other, and increased that of all the mineral dusts. The difference in the response of mineral dust and non-mineral dust INSs to (NH4)2SO4 suggests that they nucleate ice and/or interact with (NH4)2SO4 via different mechanisms.
Jingchuan Chen, Zhijun Wu, Jie Chen, Naama Reicher, Xin Fang, Yinon Rudich, and Min Hu
Atmos. Chem. Phys., 21, 3491–3506, https://doi.org/10.5194/acp-21-3491-2021, https://doi.org/10.5194/acp-21-3491-2021, 2021
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Asian mineral dust is a crucial contributor to global ice-nucleating particles (INPs), while its size-resolved information on freezing activity is extremely rare. Here we conducted the first known INP measurements of size-resolved airborne East Asian dust particles. An explicit size dependence of both INP concentration and surface
ice-active-site density was observed. The new parameterizations can be widely applied in models to better characterize and predict ice nucleation activities of dust.
Georgia Michailoudi, Jack J. Lin, Hayato Yuzawa, Masanari Nagasaka, Marko Huttula, Nobuhiro Kosugi, Theo Kurtén, Minna Patanen, and Nønne L. Prisle
Atmos. Chem. Phys., 21, 2881–2894, https://doi.org/10.5194/acp-21-2881-2021, https://doi.org/10.5194/acp-21-2881-2021, 2021
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This study provides insight into hydration of two significant atmospheric compounds, glyoxal and methylglyoxal. Using synchrotron radiation excited X-ray absorption spectroscopy, we confirm that glyoxal is fully hydrated in water, and for the first time, we experimentally detect enol structures in aqueous methylglyoxal. Our results support the contribution of these compounds to secondary organic aerosol formation, known to have a large uncertainty in atmospheric models and climate predictions.
Jianzhong Sun, Yuzhe Zhang, Guorui Zhi, Regina Hitzenberger, Wenjing Jin, Yingjun Chen, Lei Wang, Chongguo Tian, Zhengying Li, Rong Chen, Wen Xiao, Yuan Cheng, Wei Yang, Liying Yao, Yang Cao, Duo Huang, Yueyuan Qiu, Jiali Xu, Xiaofei Xia, Xin Yang, Xi Zhang, Zheng Zong, Yuchun Song, and Changdong Wu
Atmos. Chem. Phys., 21, 2329–2341, https://doi.org/10.5194/acp-21-2329-2021, https://doi.org/10.5194/acp-21-2329-2021, 2021
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Brown carbon (BrC) emission factors from household biomass fuels were measured with an integrating sphere optics approach supported by iterative calculations. A novel algorithm to directly estimate the absorption contribution of BrC relative to that of BrC + black carbon (FBrC) was proposed based purely on the absorption exponent (AAE)
(FBrC = 0.5519 lnAAE + 0.0067). The FBrC for household biomass fuels was as high as 50.8 % across the strongest solar spectral range of 350−850 nm.
Weigang Wang, Ting Lei, Andreas Zuend, Hang Su, Yafang Cheng, Yajun Shi, Maofa Ge, and Mingyuan Liu
Atmos. Chem. Phys., 21, 2179–2190, https://doi.org/10.5194/acp-21-2179-2021, https://doi.org/10.5194/acp-21-2179-2021, 2021
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Aerosol mixing state regulates the interactions between water molecules and particles and thus controls aerosol activation and hygroscopic growth, which thereby influences visibility degradation, cloud formation, and its radiative forcing. However, there are few studies attempting to investigate their interactions with water molecules. Here, we investigated the effect of organic coatings on the hygroscopic behavior of the inorganic core.
Sabin Kasparoglu, Ying Li, Manabu Shiraiwa, and Markus D. Petters
Atmos. Chem. Phys., 21, 1127–1141, https://doi.org/10.5194/acp-21-1127-2021, https://doi.org/10.5194/acp-21-1127-2021, 2021
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Viscosity is important because it determines the lifetime, impact, and fate of particulate matter. We collected new data to rigorously test a framework that is used to constrain the phase state in global simulations. We find that the framework is accurate as long as appropriate compound specific inputs are available.
Cuiqi Zhang, Yue Zhang, Martin J. Wolf, Leonid Nichman, Chuanyang Shen, Timothy B. Onasch, Longfei Chen, and Daniel J. Cziczo
Atmos. Chem. Phys., 20, 13957–13984, https://doi.org/10.5194/acp-20-13957-2020, https://doi.org/10.5194/acp-20-13957-2020, 2020
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Black carbon (BC) is considered the second most important global warming agent. However, the role of BC aerosol–cloud–climate interactions in the cirrus formation remains uncertain. Our study of selected BC types and sizes suggests that increases in diameter, compactness, and/or surface oxidation of BC particles lead to more efficient ice nucleation (IN) via pore condensation freezing (PCF) pathways，and that coatings of common secondary organic aerosol (SOA) materials can inhibit ice formation.
Luisa Ickes, Grace C. E. Porter, Robert Wagner, Michael P. Adams, Sascha Bierbauer, Allan K. Bertram, Merete Bilde, Sigurd Christiansen, Annica M. L. Ekman, Elena Gorokhova, Kristina Höhler, Alexei A. Kiselev, Caroline Leck, Ottmar Möhler, Benjamin J. Murray, Thea Schiebel, Romy Ullrich, and Matthew E. Salter
Atmos. Chem. Phys., 20, 11089–11117, https://doi.org/10.5194/acp-20-11089-2020, https://doi.org/10.5194/acp-20-11089-2020, 2020
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The Arctic is a region where aerosols are scarce. Sea spray might be a potential source of aerosols acting as ice-nucleating particles. We investigate two common phytoplankton species (Melosira arctica and Skeletonema marinoi) and present their ice nucleation activity in comparison with Arctic seawater microlayer samples from different field campaigns. We also aim to understand the aerosolization process of marine biological samples and the potential effect on the ice nucleation activity.
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.
Damon M. Smith, Marc N. Fiddler, Rudra P. Pokhrel, and Solomon Bililign
Atmos. Chem. Phys., 20, 10149–10168, https://doi.org/10.5194/acp-20-10149-2020, https://doi.org/10.5194/acp-20-10149-2020, 2020
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Biomass burning aerosol can scatter and absorb light, contributing to the cooling or warming of the planet. The scattering and absorption properties (optical properties) change as aerosol ages and interacts with atmospheric gases. Optical properties also depend on burning conditions, fuel type, and morphology. Africa is a major source of biomass burning aerosols, but there are very few laboratory studies. This study focuses on the optical properties of aerosols from east African biomass fuels.
Dominik Stolzenburg, Mario Simon, Ananth Ranjithkumar, Andreas Kürten, Katrianne Lehtipalo, Hamish Gordon, Sebastian Ehrhart, Henning Finkenzeller, Lukas Pichelstorfer, Tuomo Nieminen, Xu-Cheng He, Sophia Brilke, Mao Xiao, António Amorim, Rima Baalbaki, Andrea Baccarini, Lisa Beck, Steffen Bräkling, Lucía Caudillo Murillo, Dexian Chen, Biwu Chu, Lubna Dada, António Dias, Josef Dommen, Jonathan Duplissy, Imad El Haddad, Lukas Fischer, Loic Gonzalez Carracedo, Martin Heinritzi, Changhyuk Kim, Theodore K. Koenig, Weimeng Kong, Houssni Lamkaddam, Chuan Ping Lee, Markus Leiminger, Zijun Li, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Tatjana Müller, Wei Nie, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Matti P. Rissanen, Birte Rörup, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Mingyi Wang, Yonghong Wang, Stefan K. Weber, Daniela Wimmer, Peter J. Wlasits, Yusheng Wu, Qing Ye, Marcel Zauner-Wieczorek, Urs Baltensperger, Kenneth S. Carslaw, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Armin Hansel, Markku Kulmala, Jos Lelieveld, Rainer Volkamer, Jasper Kirkby, and Paul M. Winkler
Atmos. Chem. Phys., 20, 7359–7372, https://doi.org/10.5194/acp-20-7359-2020, https://doi.org/10.5194/acp-20-7359-2020, 2020
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Sulfuric acid is a major atmospheric vapour for aerosol formation. If new particles grow fast enough, they can act as cloud droplet seeds or affect air quality. In a controlled laboratory set-up, we demonstrate that van der Waals forces enhance growth from sulfuric acid. We disentangle the effects of ammonia, ions and particle hydration, presenting a complete picture of sulfuric acid growth from molecular clusters onwards. In a climate model, we show its influence on the global aerosol budget.
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.
Wenyu Zhang, Weigang Wang, Junling Li, Chao Peng, Kun Li, Li Zhou, Bo Shi, Yan Chen, Mingyuan Liu, and Maofa Ge
Atmos. Chem. Phys., 20, 4477–4492, https://doi.org/10.5194/acp-20-4477-2020, https://doi.org/10.5194/acp-20-4477-2020, 2020
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We investigated the effect of SO2 under different humidities on optical properties of toluene-derived SOA under four conditions with CRDs and PAX at 532 and 375 nm, respectively. Our results showed that SO2 under different humidities can change the refractive complex index of toluene SOA by influencing the multiphase processes and altering the aerosol chemical compositions. Different atmospheric conditions could affect the properties of toluene SOA, as well as the global radiative balance.
Junteng Wu, Alessandro Faccinetto, Symphorien Grimonprez, Sébastien Batut, Jérôme Yon, Pascale Desgroux, and Denis Petitprez
Atmos. Chem. Phys., 20, 4209–4225, https://doi.org/10.5194/acp-20-4209-2020, https://doi.org/10.5194/acp-20-4209-2020, 2020
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Soot particles released during anthropogenic activities may lead to positive direct or negative indirect climate forcing depending on their aging in the atmosphere. The latter occurs whenever soot particles act as cloud condensation nuclei (CCN) and trigger the formation of persistent clouds. Herein, we investigate the impact of the size distribution and morphology of freshly emitted soot particles on their aging process and propose a model to quantitatively predict their efficiency as CCN.
Otso Peräkylä, Matthieu Riva, Liine Heikkinen, Lauriane Quéléver, Pontus Roldin, and Mikael Ehn
Atmos. Chem. Phys., 20, 649–669, https://doi.org/10.5194/acp-20-649-2020, https://doi.org/10.5194/acp-20-649-2020, 2020
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Highly oxygenated organic molecules have been suggested to form a large part of secondary organic aerosol. However, with their exotic structures, their volatilities are not well known, making their exact role in particle formation hard to assess. In laboratory experiments, we found the volatility of HOMs formed in the ozonolysis of the monoterpene alpha-pinene to be in the middle of earlier estimates. The volatilities of HOMs could be well explained in terms of their molecular formulae.
Joel C. Corbin and Martin Gysel-Beer
Atmos. Chem. Phys., 19, 15673–15690, https://doi.org/10.5194/acp-19-15673-2019, https://doi.org/10.5194/acp-19-15673-2019, 2019
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We review the literature to refine the definition of "tar balls" (or tar particles). Then, using a marine-engine data set, we show that a standard SP2 can identify tar particles in two ways, as evaporating and non-incandescing (30 % of tar particles by number) or incandescing particles which scatter more light than soot at incandescence (70 % of tar particles by number). To our knowledge, no other technique can provide in situ, real-time evidence for the presence of tar particles in an aerosol.
Claudia Di Biagio, Paola Formenti, Yves Balkanski, Lorenzo Caponi, Mathieu Cazaunau, Edouard Pangui, Emilie Journet, Sophie Nowak, Meinrat O. Andreae, Konrad Kandler, Thuraya Saeed, Stuart Piketh, David Seibert, Earle Williams, and Jean-François Doussin
Atmos. Chem. Phys., 19, 15503–15531, https://doi.org/10.5194/acp-19-15503-2019, https://doi.org/10.5194/acp-19-15503-2019, 2019
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This paper presents a new dataset of laboratory measurements of the shortwave (SW) spectral complex refractive index and single-scattering albedo (SSA) for global mineral dust aerosols of varying origin and composition. Our results show that the dust refractive index and SSA vary strongly from source to source, mostly due to particle iron content changes. We recommend that source-dependent values of the SW spectral refractive index and SSA be used in models and remote sensing applications.
Courtney D. Hatch, Paul R. Tumminello, Megan A. Cassingham, Ann L. Greenaway, Rebecca Meredith, and Matthew J. Christie
Atmos. Chem. Phys., 19, 13581–13589, https://doi.org/10.5194/acp-19-13581-2019, https://doi.org/10.5194/acp-19-13581-2019, 2019
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Atmospheric mineral dust has been identified as an important contributor to cloud formation and cloud properties that influence the Earth's climate, yet experimental measurements of climate model parameters currently disagree. This study demonstrates current best practices for analyzing water adsorption measurements, resulting in significantly improved agreement among experimental practices. As such, more accurate parameters can be used to improve simulations of aerosol climate effects.
Mijung Song, Adrian M. Maclean, Yuanzhou Huang, Natalie R. Smith, Sandra L. Blair, Julia Laskin, Alexander Laskin, Wing-Sy Wong DeRieux, Ying Li, Manabu Shiraiwa, Sergey A. Nizkorodov, and Allan K. Bertram
Atmos. Chem. Phys., 19, 12515–12529, https://doi.org/10.5194/acp-19-12515-2019, https://doi.org/10.5194/acp-19-12515-2019, 2019
Leonid Nichman, Martin Wolf, Paul Davidovits, Timothy B. Onasch, Yue Zhang, Doug R. Worsnop, Janarjan Bhandari, Claudio Mazzoleni, and Daniel J. Cziczo
Atmos. Chem. Phys., 19, 12175–12194, https://doi.org/10.5194/acp-19-12175-2019, https://doi.org/10.5194/acp-19-12175-2019, 2019
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Previous studies showed widespread ice nucleation activity of soot. In this systematic study we investigated the factors that affect the heterogeneous ice nucleation activity of soot surrogates in the cirrus cloud regime. Our observations are consistent with an ice nucleation mechanism of pore condensation followed by freezing. The results show significant variations in ice nucleation activity as a function of size, morphology, and surface chemistry of the black-carbon-containing particles.
Martin Schnaiter, Claudia Linke, Inas Ibrahim, Alexei Kiselev, Fritz Waitz, Thomas Leisner, Stefan Norra, and Till Rehm
Atmos. Chem. Phys., 19, 10829–10844, https://doi.org/10.5194/acp-19-10829-2019, https://doi.org/10.5194/acp-19-10829-2019, 2019
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When combustion particles are deposited to the ground, they darken Earth's snow and ice surfaces by even tiny quantities. This darkening reduces the back reflection of sunlight and induces an additional climate warming. Particles from fresh snow samples were investigated according to their light absorption strength. Enhanced absorption was found in the snow that cannot fully be attributed to combustion particles. Dust and biogenic matter are likely the cause of this additional snow darkening.
Olli-Pekka Tikkanen, Väinö Hämäläinen, Grazia Rovelli, Antti Lipponen, Manabu Shiraiwa, Jonathan P. Reid, Kari E. J. Lehtinen, and Taina Yli-Juuti
Atmos. Chem. Phys., 19, 9333–9350, https://doi.org/10.5194/acp-19-9333-2019, https://doi.org/10.5194/acp-19-9333-2019, 2019
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We assessed how well the organic aerosol particle composition and viscosity can be captured by optimizing process models to match particle evaporation data. We performed the analysis for both artificial and real evaporation data and tested two optimization algorithms. Our findings show that the optimization method yields a good estimate for the studied properties. The timescale of the evaporation data and particle size was found to be important in identifying the volatility of organic compounds.
Miska Olin, Jenni Alanen, Marja R. T. Palmroth, Topi Rönkkö, and Miikka Dal Maso
Atmos. Chem. Phys., 19, 6367–6388, https://doi.org/10.5194/acp-19-6367-2019, https://doi.org/10.5194/acp-19-6367-2019, 2019
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The mechanism for new particle formation (NPF) in vehicle exhaust is currently unknown. This study focuses on determining the NPF rate in vehicle exhaust caused by sulfuric acid, which is the most promising candidate involved in the NPF process. The NPF rate function obtained in this study helps in examining the NPF mechanism in exhaust plumes, and it can also be used to improve air quality models. The results also imply that the NPF process cannot be fully explained by sulfuric acid only.
Elena C. Maters, Donald B. Dingwell, Corrado Cimarelli, Dirk Müller, Thomas F. Whale, and Benjamin J. Murray
Atmos. Chem. Phys., 19, 5451–5465, https://doi.org/10.5194/acp-19-5451-2019, https://doi.org/10.5194/acp-19-5451-2019, 2019
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This experimental study investigates the influence of volcanic ash chemical composition, crystallinity, and mineralogy on its ability to promote freezing of supercooled water. The results indicate that crystals in ash play a key role in this process and suggest that feldspars and perhaps pyroxenes in ash may be highly ice-active. These findings contribute to improving understanding of the potential of ash emissions from different explosive eruptions to impact ice formation in the atmosphere.
Zamin A. Kanji, Ryan C. Sullivan, Monika Niemand, Paul J. DeMott, Anthony J. Prenni, Cédric Chou, Harald Saathoff, and Ottmar Möhler
Atmos. Chem. Phys., 19, 5091–5110, https://doi.org/10.5194/acp-19-5091-2019, https://doi.org/10.5194/acp-19-5091-2019, 2019
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The ice nucleation ability of two natural desert dusts coated with a proxy of secondary organic aerosol is presented for temperatures and relative humidity conditions relevant for mixed-phase clouds. We find that at the tested conditions, there is no effect on the ice nucleation ability of the particles due to the organic coating. Furthermore, the two dust samples do not show variability within measurement uncertainty. Particle size and surface area may play a role in any difference observed.
Nønne L. Prisle, Jack J. Lin, Sara Purdue, Haisheng Lin, J. Carson Meredith, and Athanasios Nenes
Atmos. Chem. Phys., 19, 4741–4761, https://doi.org/10.5194/acp-19-4741-2019, https://doi.org/10.5194/acp-19-4741-2019, 2019
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We measure surface activity and cloud-forming potential of pollenkitt, an organic mixture coating pollen grains. Cloud droplet formation is affected through both surface tension and bulk depletion, with a consistent particle size-dependent signature. We observe nonideal solution effects in pollenkitt mixtures with ammonium sulfate salt. Our results suggest sensitivity of general water interactions, including cloud formation by pollen and their fragments, to both atmospheric humidity and aging.
Zhicong Yin, Huijun Wang, Yuyan Li, Xiaohui Ma, and Xinyu Zhang
Atmos. Chem. Phys., 19, 3857–3871, https://doi.org/10.5194/acp-19-3857-2019, https://doi.org/10.5194/acp-19-3857-2019, 2019
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Summer surface ozone pollution has rapidly intensified recently, damaging human and ecosystem health. This study aims to examine the large-scale atmospheric circulations associated with the interannual variation in summer surface O3 pollution in North China based on long-term meteorological observations. The impacts of Arctic sea ice were also revealed. The outcomes may provide a basis for understanding the interannual variation of 03 pollution and its seasonal to interannual prediction.
Ankit Tandon, Nicholas E. Rothfuss, and Markus D. Petters
Atmos. Chem. Phys., 19, 3325–3339, https://doi.org/10.5194/acp-19-3325-2019, https://doi.org/10.5194/acp-19-3325-2019, 2019
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Organic compounds may form a barrier to condensation. Such barriers have been hypothesized to prevent water and other substances from mixing with salt cores. This will hinder the particles' ability to aid cloud formation of < 100 nm particles. Here we perform experiments encasing particles in plastic shells akin to water bottles. Against expectations, the plastic shell did not alter the droplet activation behavior of the encased particles. Water appears to readily permeate the plastic shell.
James F. Davies, Andreas Zuend, and Kevin R. Wilson
Atmos. Chem. Phys., 19, 2933–2946, https://doi.org/10.5194/acp-19-2933-2019, https://doi.org/10.5194/acp-19-2933-2019, 2019
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The formation of cloud droplets involves the condensation of water onto preexisting particles in the atmosphere. The efficiency of this process depends on the nature of the particles, and recent work has shown that organic-rich particles may exhibit a suppressed surface tension that promotes the formation of cloud droplets. In this technical note, we discuss the mechanism for this and highlight the evolution of surface tension as the key factor in the extent of surface effects.
Nathan J. Janechek, Rachel F. Marek, Nathan Bryngelson, Ashish Singh, Robert L. Bullard, William H. Brune, and Charles O. Stanier
Atmos. Chem. Phys., 19, 1649–1664, https://doi.org/10.5194/acp-19-1649-2019, https://doi.org/10.5194/acp-19-1649-2019, 2019
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Cyclic volatile methyl siloxanes (cVMSs) are widely used chemicals in personal care products which can undergo oxidation to generate secondary organic aerosol. In this work, cVMS oxidation aerosols were generated using a photochemical chamber and the physical properties characterized. The aerosol yield, volatility, hygroscopicity, morphology, elemental composition, and proposed parameters for treatment as secondary organic aerosol in atmospheric models are provided.
Jian Wang, John E. Shilling, Jiumeng Liu, Alla Zelenyuk, David M. Bell, Markus D. Petters, Ryan Thalman, Fan Mei, Rahul A. Zaveri, and Guangjie Zheng
Atmos. Chem. Phys., 19, 941–954, https://doi.org/10.5194/acp-19-941-2019, https://doi.org/10.5194/acp-19-941-2019, 2019
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Earlier studies showed organic hygroscopicity increases with oxidation level. Such increases have been attributed to higher water solubility for more oxidized organics. By systematically varying the water content of activating droplets, we show that for secondary organic aerosols, essentially all organics are dissolved at the point of droplet activation. Therefore, the organic hygroscopicity is not limited by solubility but is dictated mainly by the molecular weight of organic species.
Nivedita K. Kumar, Joel C. Corbin, Emily A. Bruns, Dario Massabó, Jay G. Slowik, Luka Drinovec, Griša Močnik, Paolo Prati, Athanasia Vlachou, Urs Baltensperger, Martin Gysel, Imad El-Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 18, 17843–17861, https://doi.org/10.5194/acp-18-17843-2018, https://doi.org/10.5194/acp-18-17843-2018, 2018
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It is clear that considerable uncertainties still exist in understanding the magnitude of aerosol absorption on a global scale and its contribution to global warming. This manuscript provides a comprehensive assessment of the optical absorption by organic aerosols (brown carbon) from residential wood combustion as a function of atmospheric aging.
Yue Peng, Hong Wang, Yubin Li, Changwei Liu, Tianliang Zhao, Xiaoye Zhang, Zhiqiu Gao, Tong Jiang, Huizheng Che, and Meng Zhang
Atmos. Chem. Phys., 18, 17421–17435, https://doi.org/10.5194/acp-18-17421-2018, https://doi.org/10.5194/acp-18-17421-2018, 2018
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Two surface layer schemes are evaluated in eastern China based on observational flux data. The results indicate that the Li scheme better describes regional atmosphere stratification compared with the MM5 scheme, especially for the transition stage from unstable to stable atmosphere conditions, corresponding to PM2.5 accumulation. Our research suggests the potential improved possibilities for severe haze prediction in eastern China by coupling Li online into atmosphere chemical models.
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.
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.
Sara D. Forestieri, Taylor M. Helgestad, Andrew T. Lambe, Lindsay Renbaum-Wolff, Daniel A. Lack, Paola Massoli, Eben S. Cross, Manvendra K. Dubey, Claudio Mazzoleni, Jason S. Olfert, Arthur J. Sedlacek III, Andrew Freedman, Paul Davidovits, Timothy B. Onasch, and Christopher D. Cappa
Atmos. Chem. Phys., 18, 12141–12159, https://doi.org/10.5194/acp-18-12141-2018, https://doi.org/10.5194/acp-18-12141-2018, 2018
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We characterized optical properties of flame-derived black carbon particles and interpret our observations through the use of Mie theory and Rayleigh–Debye–Gans theory. We determined that the mass absorption coefficient is independent of particle collapse and use this to derive theory- and wavelength-specific refractive indices for black carbon (BC). We demonstrate the inadequacy of Mie theory and suggest an alternative approach for atmospheric models to better represent light absorption by BC.
Mijung Song, Suhan Ham, Ryan J. Andrews, Yuan You, and Allan K. Bertram
Atmos. Chem. Phys., 18, 12075–12084, https://doi.org/10.5194/acp-18-12075-2018, https://doi.org/10.5194/acp-18-12075-2018, 2018
Sara D. Forestieri, Sean M. Staudt, Thomas M. Kuborn, Katharine Faber, Christopher R. Ruehl, Timothy H. Bertram, and Christopher D. Cappa
Atmos. Chem. Phys., 18, 10985–11005, https://doi.org/10.5194/acp-18-10985-2018, https://doi.org/10.5194/acp-18-10985-2018, 2018
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Our work establishes how surface tension reduction influences droplet growth and activation of simple sea spray mimics (NaCl coated with fatty acids). Fatty acids can substantially reduce droplet surface tension near activation but have limited impact on activation. Coating of NaCl by palmitic acid (a wax) impedes water uptake, but this impedance is removed if oleic acid (a liquid) is mixed in. The properties that surface-active compounds need to impact activation are theoretically examined.
Cited articles
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Hoose, C. and Möhler, O.: Heterogeneous ice nucleation on atmospheric aerosols: a review of results from laboratory experiments, Atmos. Chem. Phys., 12, 9817–9854, https://doi.org/10.5194/acp-12-9817-2012, 2012.
Hoyle, C. R., Pinti, V., Welti, A., Zobrist, B., Marcolli, C., Luo, B., Höskuldsson, Á., Mattsson, H. B., Stetzer, O., Thorsteinsson, T., Larsen, G., and Peter, T.: Ice nucleation properties of volcanic ash from Eyjafjallajökull, Atmos. Chem. Phys., 11, 9911–9926, https://doi.org/10.5194/acp-11-9911-2011, 2011.
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Kulkarni, G. and Dobbie, S.: Ice nucleation properties of mineral dust particles: determination of onset RHi, IN active fraction, nucleation time-lag, and the effect of active sites on contact angles, Atmos. Chem. Phys., 10, 95–105, https://doi.org/10.5194/acp-10-95-2010, 2010.
Ladino, L., Stetzer, O., Lüönd, F., Welti, A., and Lohmann, U.: Contact freezing experiments of kaolinite particles with cloud droplets, J. Geophys. Res.-Atmos., 116, D22202, https://doi.org/10.1029/2011jd015727, 2011.
Ladino Moreno, L. A., Stetzer, O., and Lohmann, U.: Contact freezing: a review of experimental studies, Atmos. Chem. Phys., 13, 9745–9769, https://doi.org/10.5194/acp-13-9745-2013, 2013.
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Marcolli, C., Gedamke, S., Peter, T., and Zobrist, B.: Efficiency of immersion mode ice nucleation on surrogates of mineral dust, Atmos. Chem. Phys., 7, 5081–5091, https://doi.org/10.5194/acp-7-5081-2007, 2007.
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Murray, B. J., Broadley, S. L., Wilson, T. W., Atkinson, J. D., and Wills, R. H.: Heterogeneous freezing of water droplets containing kaolinite particles, Atmos. Chem. Phys., 11, 4191–4207, https://doi.org/10.5194/acp-11-4191-2011, 2011.
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