Articles | Volume 15, issue 23
https://doi.org/10.5194/amt-15-7137-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/amt-15-7137-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
12 Dec 2022
Research article |
| 12 Dec 2022
| 12 Dec 2022
Mass spectrometry-based Aerosolomics: a new approach to resolve sources, composition, and partitioning of secondary organic aerosol
Institute for Atmospheric and Environmental Sciences, Goethe-University Frankfurt, 60438 Frankfurt am Main, Germany
Franziska Bachmeier
Institute for Atmospheric and Environmental Sciences, Goethe-University Frankfurt, 60438 Frankfurt am Main, Germany
Felix Leonard Gottwald
Institute for Atmospheric and Environmental Sciences, Goethe-University Frankfurt, 60438 Frankfurt am Main, Germany
Mario Simon
Institute for Atmospheric and Environmental Sciences, Goethe-University Frankfurt, 60438 Frankfurt am Main, Germany
Alexander Lucas Vogel
CORRESPONDING AUTHOR
Institute for Atmospheric and Environmental Sciences, Goethe-University Frankfurt, 60438 Frankfurt am Main, Germany
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Florian Ungeheuer, Dominik van Pinxteren, and Alexander L. Vogel
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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
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Mario Simon, Lubna Dada, Martin Heinritzi, Wiebke Scholz, Dominik Stolzenburg, Lukas Fischer, Andrea C. Wagner, Andreas Kürten, Birte Rörup, Xu-Cheng He, João Almeida, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Lisa Beck, Anton Bergen, Federico Bianchi, Steffen Bräkling, Sophia Brilke, Lucia Caudillo, Dexian Chen, Biwu Chu, António Dias, Danielle C. Draper, Jonathan Duplissy, Imad El-Haddad, Henning Finkenzeller, Carla Frege, Loic Gonzalez-Carracedo, Hamish Gordon, Manuel Granzin, Jani Hakala, Victoria Hofbauer, Christopher R. Hoyle, Changhyuk Kim, Weimeng Kong, Houssni Lamkaddam, Chuan P. Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Bernhard Mentler, Ugo Molteni, Leonid Nichman, Wei Nie, Andrea Ojdanic, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Lauriane L. J. Quéléver, Ananth Ranjithkumar, Matti P. Rissanen, Simon Schallhart, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee J. Tham, António R. Tomé, Miguel Vazquez-Pufleau, Alexander L. Vogel, Robert Wagner, Mingyi Wang, Dongyu S. Wang, Yonghong Wang, Stefan K. Weber, Yusheng Wu, Mao Xiao, Chao Yan, Penglin Ye, Qing Ye, Marcel Zauner-Wieczorek, Xueqin Zhou, Urs Baltensperger, Josef Dommen, Richard C. Flagan, Armin Hansel, Markku Kulmala, Rainer Volkamer, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 9183–9207, https://doi.org/10.5194/acp-20-9183-2020, https://doi.org/10.5194/acp-20-9183-2020, 2020
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Highly oxygenated organic compounds (HOMs) have been identified as key vapors involved in atmospheric new-particle formation (NPF). The molecular distribution, HOM yield, and NPF from α-pinene oxidation experiments were measured at the CLOUD chamber over a wide tropospheric-temperature range. This study shows on a molecular scale that despite the sharp reduction in HOM yield at lower temperatures, the reduced volatility counteracts this effect and leads to an overall increase in the NPF rate.
Lu Qi, Alexander L. Vogel, Sepideh Esmaeilirad, Liming Cao, Jing Zheng, Jean-Luc Jaffrezo, Paola Fermo, Anne Kasper-Giebl, Kaspar R. Daellenbach, Mindong Chen, Xinlei Ge, Urs Baltensperger, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 20, 7875–7893, https://doi.org/10.5194/acp-20-7875-2020, https://doi.org/10.5194/acp-20-7875-2020, 2020
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We present the first application of this online and offline strategy using the new extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF), which achieves increased chemical specificity relative to other online techniques. Measurement and source apportionment of 1 year of filter samples collected in Zurich, Switzerland, show seasonal contributions from fresh and aged wood combustion in winter and biogenic emission-derived SOA in summer, as well as other sources.
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.
Joschka Pfeifer, Mario Simon, Martin Heinritzi, Felix Piel, Lena Weitz, Dongyu Wang, Manuel Granzin, Tatjana Müller, Steffen Bräkling, Jasper Kirkby, Joachim Curtius, and Andreas Kürten
Atmos. Meas. Tech., 13, 2501–2522, https://doi.org/10.5194/amt-13-2501-2020, https://doi.org/10.5194/amt-13-2501-2020, 2020
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Ammonia is an important atmospheric trace gas that affects secondary aerosol formation and, together with sulfuric acid, the formation of new particles. A measurement technique is presented that uses high-resolution mass spectrometry and protonated water clusters for the ultrasensitive detection of ammonia at single-digit parts per trillion by volume levels. The instrument is further capable of measuring amines and a suite of iodine compounds at sub-parts per trillion by volume levels.
Kaspar R. Daellenbach, Ivan Kourtchev, Alexander L. Vogel, Emily A. Bruns, Jianhui Jiang, Tuukka Petäjä, Jean-Luc Jaffrezo, Sebnem Aksoyoglu, Markus Kalberer, Urs Baltensperger, Imad El Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 19, 5973–5991, https://doi.org/10.5194/acp-19-5973-2019, https://doi.org/10.5194/acp-19-5973-2019, 2019
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Here we present the molecular composition of the organic aerosol (OA) at an urban site in Central Europe (Zurich, Switzerland) and compare it to smog chamber wood smoke and ambient biogenic secondary OA (SOA) (Orbitrap analyses). Accordingly, we are able to explain the strong seasonality of the molecular composition by aged wood smoke and biogenic SOA during winter and summer. Our results could also explain the predominance of non-fossil organic carbon at European locations throughout the year.
Andrea C. Wagner, Anton Bergen, Sophia Brilke, Claudia Fuchs, Markus Ernst, Jesica Hoker, Martin Heinritzi, Mario Simon, Bertram Bühner, Joachim Curtius, and Andreas Kürten
Atmos. Meas. Tech., 11, 5489–5506, https://doi.org/10.5194/amt-11-5489-2018, https://doi.org/10.5194/amt-11-5489-2018, 2018
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Chemical analysis of sub-30 nm aerosol particles is important for understanding aerosol nucleation and early growth, yet it is still an experimental challenge. In this study, we present a novel device for size resolved chemical analysis of nucleation and Aitken mode particles (from ~10 to ~30 nm) while allowing gas phase measurements with the same detector. Particles are charged, size selected, electrostatically collected and then thermally desorbed in a carrier gas.
Andreas Kürten, Chenxi Li, Federico Bianchi, Joachim Curtius, António Dias, Neil M. Donahue, Jonathan Duplissy, Richard C. Flagan, Jani Hakala, Tuija Jokinen, Jasper Kirkby, Markku Kulmala, Ari Laaksonen, Katrianne Lehtipalo, Vladimir Makhmutov, Antti Onnela, Matti P. Rissanen, Mario Simon, Mikko Sipilä, Yuri Stozhkov, Jasmin Tröstl, Penglin Ye, and Peter H. McMurry
Atmos. Chem. Phys., 18, 845–863, https://doi.org/10.5194/acp-18-845-2018, https://doi.org/10.5194/acp-18-845-2018, 2018
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A recent laboratory study (CLOUD) showed that new particles nucleate efficiently from sulfuric acid and dimethylamine (DMA). The reanalysis of previously published data reveals that the nucleation rates are even faster than previously assumed, i.e., nucleation can proceed at rates that are compatible with collision-controlled new particle formation for atmospheric conditions. This indicates that sulfuric acid–DMA nucleation is likely an important source of particles in the boundary layer.
Carla Frege, Ismael K. Ortega, Matti P. Rissanen, Arnaud P. Praplan, Gerhard Steiner, Martin Heinritzi, Lauri Ahonen, António Amorim, Anne-Kathrin Bernhammer, Federico Bianchi, Sophia Brilke, Martin Breitenlechner, Lubna Dada, António Dias, Jonathan Duplissy, Sebastian Ehrhart, Imad El-Haddad, Lukas Fischer, Claudia Fuchs, Olga Garmash, Marc Gonin, Armin Hansel, Christopher R. Hoyle, Tuija Jokinen, Heikki Junninen, Jasper Kirkby, Andreas Kürten, Katrianne Lehtipalo, Markus Leiminger, Roy Lee Mauldin, Ugo Molteni, Leonid Nichman, Tuukka Petäjä, Nina Sarnela, Siegfried Schobesberger, Mario Simon, Mikko Sipilä, Dominik Stolzenburg, António Tomé, Alexander L. Vogel, Andrea C. Wagner, Robert Wagner, Mao Xiao, Chao Yan, Penglin Ye, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Markku Kulmala, Douglas R. Worsnop, Paul M. Winkler, Josef Dommen, and Urs Baltensperger
Atmos. Chem. Phys., 18, 65–79, https://doi.org/10.5194/acp-18-65-2018, https://doi.org/10.5194/acp-18-65-2018, 2018
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It was recently shown that biogenic highly oxygenated molecules (HOMs) form particles in the absence of sulfuric acid and ions enhance the nucleation rate. Here we compare the molecular composition of positive and negative HOM clusters at 25, 5 and −25 °C. At lower temperatures the HOM average oxygen-to-carbon ratio decreases indicating a reduction in the rate of autoxidation due to rather high activation energy. The experimental findings are supported by quantum chemical calculations.
António Dias, Sebastian Ehrhart, Alexander Vogel, Christina Williamson, João Almeida, Jasper Kirkby, Serge Mathot, Samuel Mumford, and Antti Onnela
Atmos. Meas. Tech., 10, 5075–5088, https://doi.org/10.5194/amt-10-5075-2017, https://doi.org/10.5194/amt-10-5075-2017, 2017
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The CERN CLOUD chamber is used to understand different processes of particle formation in the atmosphere. This information can be used by global climate models to update the influence of cloud formation. To provide the most accurate information on these processes, a thorough understanding of the chamber is necessary. Temperature measurements were performed inside the entire volume of the CLOUD chamber to ensure temperature stability and more accurate estimations of particle formation parameters.
Robert Wagner, Chao Yan, Katrianne Lehtipalo, Jonathan Duplissy, Tuomo Nieminen, Juha Kangasluoma, Lauri R. Ahonen, Lubna Dada, Jenni Kontkanen, Hanna E. Manninen, Antonio Dias, Antonio Amorim, Paulus S. Bauer, Anton Bergen, Anne-Kathrin Bernhammer, Federico Bianchi, Sophia Brilke, Stephany Buenrostro Mazon, Xuemeng Chen, Danielle C. Draper, Lukas Fischer, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Jani Hakala, Liine Heikkinen, Martin Heinritzi, Victoria Hofbauer, Christopher R. Hoyle, Jasper Kirkby, Andreas Kürten, Alexander N. Kvashnin, Tiia Laurila, Michael J. Lawler, Huajun Mai, Vladimir Makhmutov, Roy L. Mauldin III, Ugo Molteni, Leonid Nichman, Wei Nie, Andrea Ojdanic, Antti Onnela, Felix Piel, Lauriane L. J. Quéléver, Matti P. Rissanen, Nina Sarnela, Simon Schallhart, Kamalika Sengupta, Mario Simon, Dominik Stolzenburg, Yuri Stozhkov, Jasmin Tröstl, Yrjö Viisanen, Alexander L. Vogel, Andrea C. Wagner, Mao Xiao, Penglin Ye, Urs Baltensperger, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Martin Gallagher, Armin Hansel, James N. Smith, António Tomé, Paul M. Winkler, Douglas Worsnop, Mikael Ehn, Mikko Sipilä, Veli-Matti Kerminen, Tuukka Petäjä, and Markku Kulmala
Atmos. Chem. Phys., 17, 15181–15197, https://doi.org/10.5194/acp-17-15181-2017, https://doi.org/10.5194/acp-17-15181-2017, 2017
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.
Andreas Kürten, Anton Bergen, Martin Heinritzi, Markus Leiminger, Verena Lorenz, Felix Piel, Mario Simon, Robert Sitals, Andrea C. Wagner, and Joachim Curtius
Atmos. Chem. Phys., 16, 12793–12813, https://doi.org/10.5194/acp-16-12793-2016, https://doi.org/10.5194/acp-16-12793-2016, 2016
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Field measurements were conducted at a rural site in central Germany close to dairy farms to investigate if there is a connection between new particle formation and the presence of amines. A variety of trace gases were measured in addition to amines, like sulfuric acid, ammonia and highly oxygenated organic molecules (HOM). The results indicate that amines are very likely involved in the growth of aerosol particles and probably also in the nucleation process, although HOM could be relevant, too.
Mario Simon, Martin Heinritzi, Stephan Herzog, Markus Leiminger, Federico Bianchi, Arnaud Praplan, Josef Dommen, Joachim Curtius, and Andreas Kürten
Atmos. Meas. Tech., 9, 2135–2145, https://doi.org/10.5194/amt-9-2135-2016, https://doi.org/10.5194/amt-9-2135-2016, 2016
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This study demonstrate the detection of dimethylamine at low mixing ratios by nitrate chemical ionization mass spectrometry (CIMS). Due to simultaneously high-sensitive gas-phase measurements of DMA, sulfuric acid, and extremely low volatile organic compounds (ELVOCs), this technique can be used as a versatile tool for studying new particle formation in the atmosphere.
Martin Heinritzi, Mario Simon, Gerhard Steiner, Andrea C. Wagner, Andreas Kürten, Armin Hansel, and Joachim Curtius
Atmos. Meas. Tech., 9, 1449–1460, https://doi.org/10.5194/amt-9-1449-2016, https://doi.org/10.5194/amt-9-1449-2016, 2016
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An easy-to-use method of estimating the mass-dependent transmission efficiency of a CIMS is presented. It makes use of depleting nitrate primary ions by different perfluorinated acids to obtain the transmission efficiency of these acids relative to the primary ion. Knowledge about the transmission efficiency is crucial for, e.g., quantification of extremely low volatile organic compounds.
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.
C. R. Hoyle, C. Fuchs, E. Järvinen, H. Saathoff, A. Dias, I. El Haddad, M. Gysel, S. C. Coburn, J. Tröstl, A.-K. Bernhammer, F. Bianchi, M. Breitenlechner, J. C. Corbin, J. Craven, N. M. Donahue, J. Duplissy, S. Ehrhart, C. Frege, H. Gordon, N. Höppel, M. Heinritzi, T. B. Kristensen, U. Molteni, L. Nichman, T. Pinterich, A. S. H. Prévôt, M. Simon, J. G. Slowik, G. Steiner, A. Tomé, A. L. Vogel, R. Volkamer, A. C. Wagner, R. Wagner, A. S. Wexler, C. Williamson, P. M. Winkler, C. Yan, A. Amorim, J. Dommen, J. Curtius, M. W. Gallagher, R. C. Flagan, A. Hansel, J. Kirkby, M. Kulmala, O. Möhler, F. Stratmann, D. R. Worsnop, and U. Baltensperger
Atmos. Chem. Phys., 16, 1693–1712, https://doi.org/10.5194/acp-16-1693-2016, https://doi.org/10.5194/acp-16-1693-2016, 2016
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A significant portion of sulphate, an important constituent of atmospheric aerosols, is formed via the aqueous phase oxidation of sulphur dioxide by ozone. The rate of this reaction has previously only been measured over a relatively small temperature range. Here, we use the state of the art CLOUD chamber at CERN to perform the first measurements of this reaction rate in super-cooled droplets, confirming that the existing extrapolation of the reaction rate to sub-zero temperatures is accurate.
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. Kürten, S. Münch, L. Rondo, F. Bianchi, J. Duplissy, T. Jokinen, H. Junninen, N. Sarnela, S. Schobesberger, M. Simon, M. Sipilä, J. Almeida, A. Amorim, J. Dommen, N. M. Donahue, E. M. Dunne, R. C. Flagan, A. Franchin, J. Kirkby, A. Kupc, V. Makhmutov, T. Petäjä, A. P. Praplan, F. Riccobono, G. Steiner, A. Tomé, G. Tsagkogeorgas, P. E. Wagner, D. Wimmer, U. Baltensperger, M. Kulmala, D. R. Worsnop, and J. Curtius
Atmos. Chem. Phys., 15, 10701–10721, https://doi.org/10.5194/acp-15-10701-2015, https://doi.org/10.5194/acp-15-10701-2015, 2015
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New particle formation (NPF) is an important atmospheric process. At cold temperatures in the upper troposphere the binary (H2SO4-H2O) and ternary (H2SO4-H2O-NH3) system are thought to be important for NPF. Sulfuric acid monomer (H2SO4) and sulfuric acid dimer ((H2SO4)2) concentrations were measured between 208 and 248K for these systems and dimer evaporation rates were derived. These data will help to better understand and predict binary and ternary nucleation at low temperatures.
A. P. Praplan, S. Schobesberger, F. Bianchi, M. P. Rissanen, M. Ehn, T. Jokinen, H. Junninen, A. Adamov, A. Amorim, J. Dommen, J. Duplissy, J. Hakala, A. Hansel, M. Heinritzi, J. Kangasluoma, J. Kirkby, M. Krapf, A. Kürten, K. Lehtipalo, F. Riccobono, L. Rondo, N. Sarnela, M. Simon, A. Tomé, J. Tröstl, P. M. Winkler, C. Williamson, P. Ye, J. Curtius, U. Baltensperger, N. M. Donahue, M. Kulmala, and D. R. Worsnop
Atmos. Chem. Phys., 15, 4145–4159, https://doi.org/10.5194/acp-15-4145-2015, https://doi.org/10.5194/acp-15-4145-2015, 2015
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Our study shows, based on data from three atmospheric pressure interface time-of-flight mass spectrometers measuring in parallel charged and neutral molecules and molecular clusters, how oxidised organic compounds bind to inorganic ions (e.g. bisulfate, nitrate, ammonium). This ionisation is selective for compounds with lower molar mass due to their limited amount and variety of functional groups. We also found that extremely low volatile organic compounds (ELVOCs) can be formed immediately.
A. L. Corrigan, L. M. Russell, S. Takahama, M. Äijälä, M. Ehn, H. Junninen, J. Rinne, T. Petäjä, M. Kulmala, A. L. Vogel, T. Hoffmann, C. J. Ebben, F. M. Geiger, P. Chhabra, J. H. Seinfeld, D. R. Worsnop, W. Song, J. Auld, and J. Williams
Atmos. Chem. Phys., 13, 12233–12256, https://doi.org/10.5194/acp-13-12233-2013, https://doi.org/10.5194/acp-13-12233-2013, 2013
A. L. Vogel, M. Äijälä, A. L. Corrigan, H. Junninen, M. Ehn, T. Petäjä, D. R. Worsnop, M. Kulmala, L. M. Russell, J. Williams, and T. Hoffmann
Atmos. Chem. Phys., 13, 10933–10950, https://doi.org/10.5194/acp-13-10933-2013, https://doi.org/10.5194/acp-13-10933-2013, 2013
A. L. Vogel, M. Äijälä, M. Brüggemann, M. Ehn, H. Junninen, T. Petäjä, D. R. Worsnop, M. Kulmala, J. Williams, and T. Hoffmann
Atmos. Meas. Tech., 6, 431–443, https://doi.org/10.5194/amt-6-431-2013, https://doi.org/10.5194/amt-6-431-2013, 2013
Related subject area
Subject: Aerosols | Technique: Laboratory Measurement | Topic: Data Processing and Information Retrieval
The role of fuel and environmental conditions on the amount and composition of primary, fresh, and aged aerosol emissions originating from diesel- and gasoline-operated auxiliary heaters of passenger cars
Estimating errors in vehicle secondary aerosol production factors due to oxidation flow reactor response time
Quantifying functional group compositions of household fuel-burning emissions
A new software toolkit for optical apportionment of carbonaceous aerosol
Theoretical derivation of aerosol lidar ratio using Mie theory for CALIOP-CALIPSO and OPAC aerosol models
An extraction method for nitrogen isotope measurement of ammonium in a low-concentration environment
Estimation of secondary organic aerosol formation parameters for the volatility basis set combining thermodenuder, isothermal dilution, and yield measurements
Characterization of offline analysis of particulate matter with FIGAERO-CIMS
A universally applicable method of calculating confidence bands for ice nucleation spectra derived from droplet freezing experiments
Thermal–optical analysis of quartz fiber filters loaded with snow samples – determination of iron based on interferences caused by mineral dust
Modelling ultrafine particle growth in a flow tube reactor
Substantial organic impurities at the surface of synthetic ammonium sulfate particles
Contrasting mineral dust abundances from X-ray diffraction and reflectance spectroscopy
Fragment ion–functional group relationships in organic aerosols using aerosol mass spectrometry and mid-infrared spectroscopy
Evolution under dark conditions of particles from old and modern diesel vehicles in a new environmental chamber characterized with fresh exhaust emissions
Quantification of isomer-resolved iodide chemical ionization mass spectrometry sensitivity and uncertainty using a voltage-scanning approach
Assessing the sources of particles at an urban background site using both regulatory instruments and low-cost sensors – a comparative study
High-resolution optical constants of crystalline ammonium nitrate for infrared remote sensing of the Asian Tropopause Aerosol Layer
Assessing the accuracy of low-cost optical particle sensors using a physics-based approach
Comparison of dimension reduction techniques in the analysis of mass spectrometry data
Development of a new correction algorithm applicable to any filter-based absorption photometer
Chemical discrimination of the particulate and gas phases of miniCAST exhausts using a two-filter collection method
External and internal cloud condensation nuclei (CCN) mixtures: controlled laboratory studies of varying mixing states
Classification of iron oxide aerosols by a single particle soot photometer using supervised machine learning
Method to measure the size-resolved real part of aerosol refractive index using differential mobility analyzer in tandem with single-particle soot photometer
Quantitative capabilities of STXM to measure spatially resolved organic volume fractions of mixed organic ∕ inorganic particles
Revisiting the differential freezing nucleus spectra derived from drop-freezing experiments: methods of calculation, applications, and confidence limits
Particle wall-loss correction methods in smog chamber experiments
Improved real-time bio-aerosol classification using artificial neural networks
Machine learning for improved data analysis of biological aerosol using the WIBS
A machine learning approach to aerosol classification for single-particle mass spectrometry
Evaluation of a hierarchical agglomerative clustering method applied to WIBS laboratory data for improved discrimination of biological particles by comparing data preparation techniques
Using depolarization to quantify ice nucleating particle concentrations: a new method
Real-time analysis of insoluble particles in glacial ice using single-particle mass spectrometry
Evaluation of machine learning algorithms for classification of primary biological aerosol using a new UV-LIF spectrometer
Size distribution of particle-associated polybrominated diphenyl ethers (PBDEs) and their implications for health
Predicting ambient aerosol thermal–optical reflectance (TOR) measurements from infrared spectra: extending the predictions to different years and different sites
Electrodynamic balance measurements of thermodynamic, kinetic, and optical aerosol properties inaccessible to bulk methods
Mass-specific optical absorption coefficients and imaginary part of the complex refractive indices of mineral dust components measured by a multi-wavelength photoacoustic spectrometer
An experiment to measure raindrop collection efficiencies: influence of rear capture
Quantitative single-particle analysis with the Aerodyne aerosol mass spectrometer: development of a new classification algorithm and its application to field data
A modeling approach to evaluate the uncertainty in estimating the evaporation behaviour and volatility of organic aerosols
A model of aerosol evaporation kinetics in a thermodenuder
Henri Oikarinen, Anni Hartikainen, Pauli Simonen, Miska Olin, Ukko-Ville Mäkinen, Petteri Marjanen, Laura Salo, Ville Silvonen, Sampsa Martikainen, Jussi Hoivala, Mika Ihalainen, Pasi Miettinen, Pasi Yli-Pirilä, Olli Sippula, Santtu Mikkonen, and Panu Karjalainen
EGUsphere, https://doi.org/10.5194/egusphere-2025-540, https://doi.org/10.5194/egusphere-2025-540, 2025
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Fuel-operated auxiliary heaters are used in vehicles to provide extra heating to improve passenger comfort and vehicle functionality in cold climates. Currently heater emissions are not regulated as part of vehicle emissions, so this research was done to assess harmful gaseous and airborne particle emissions from them. Heaters were found to be major source of particles, especially when particles formed after combustion were accounted for, and large carbon monoxide emissions were also observed.
Pauli Simonen, Miikka Dal Maso, Pinja Prauda, Anniina Hoilijoki, Anette Karppinen, Pekka Matilainen, Panu Karjalainen, and Jorma Keskinen
Atmos. Meas. Tech., 17, 3219–3236, https://doi.org/10.5194/amt-17-3219-2024, https://doi.org/10.5194/amt-17-3219-2024, 2024
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Secondary aerosol is formed in the atmosphere from gaseous emissions. Oxidation flow reactors used in secondary aerosol research do not immediately respond to changes in the inlet concentration of gases because of their broad transfer functions. This may result in incorrect secondary aerosol production factors determined for vehicles. We studied the extent of possible errors and found that oxidation flow reactors with faster responses result in smaller errors.
Emily Y. Li, Amir Yazdani, Ann M. Dillner, Guofeng Shen, Wyatt M. Champion, James J. Jetter, William T. Preston, Lynn M. Russell, Michael D. Hays, and Satoshi Takahama
Atmos. Meas. Tech., 17, 2401–2413, https://doi.org/10.5194/amt-17-2401-2024, https://doi.org/10.5194/amt-17-2401-2024, 2024
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Infrared spectroscopy is a cost-effective measurement technique to characterize the chemical composition of organic aerosol emissions. This technique differentiates the organic matter emission factor from different fuel sources by their characteristic functional groups. Comparison with collocated measurements suggests that polycyclic aromatic hydrocarbon concentrations in emissions estimated by conventional chromatography may be substantially underestimated.
Tommaso Isolabella, Vera Bernardoni, Alessandro Bigi, Marco Brunoldi, Federico Mazzei, Franco Parodi, Paolo Prati, Virginia Vernocchi, and Dario Massabò
Atmos. Meas. Tech., 17, 1363–1373, https://doi.org/10.5194/amt-17-1363-2024, https://doi.org/10.5194/amt-17-1363-2024, 2024
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We present an innovative software toolkit to differentiate sources of carbonaceous aerosol in the atmosphere. Our toolkit implements an upgraded mathematical model which allows for determination of fundamental optical properties of the aerosol, its sources, and the mass concentration of different carbonaceous species of particulate matter. We have tested the functionality of the software by re-analysing published data, and we obtained a compatible results with additional information.
Radhika A. Chipade and Mehul R. Pandya
Atmos. Meas. Tech., 16, 5443–5459, https://doi.org/10.5194/amt-16-5443-2023, https://doi.org/10.5194/amt-16-5443-2023, 2023
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The extinction-to-backscattering ratio, popularly known as lidar ratio of atmospheric aerosols, is an important optical property, which is essential to retrieve the extinction profiles of atmospheric aerosols. A physics-based theoretical approach is presented in the present paper that estimates lidar ratio values for CALIPSO and OPAC aerosol models, which can be used as inputs to determine the extinction profiles of aerosols using CALIPSO data.
Alexis Lamothe, Joel Savarino, Patrick Ginot, Lison Soussaintjean, Elsa Gautier, Pete D. Akers, Nicolas Caillon, and Joseph Erbland
Atmos. Meas. Tech., 16, 4015–4030, https://doi.org/10.5194/amt-16-4015-2023, https://doi.org/10.5194/amt-16-4015-2023, 2023
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Ammonia is a reactive gas in our atmosphere that is key in air quality issues. Assessing its emissions and how it reacts is a hot topic that can be addressed from the past. Stable isotopes (the mass of the molecule) measured in ice cores (glacial archives) can teach us a lot. However, the concentrations in ice cores are very small. We propose a protocol to limit the contamination and apply it to one ice core drilled in Mont Blanc, describing the opportunities our method brings.
Petro Uruci, Dontavious Sippial, Anthoula Drosatou, and Spyros N. Pandis
Atmos. Meas. Tech., 16, 3155–3172, https://doi.org/10.5194/amt-16-3155-2023, https://doi.org/10.5194/amt-16-3155-2023, 2023
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In this work we develop an algorithm for the synthesis of the measurements performed in atmospheric simulation chambers regarding the formation of secondary organic aerosol (SOA). Novel features of the algorithm are its ability to use measurements of SOA yields, thermodenuders, and isothermal dilution; its estimation of parameters that can be used directly in atmospheric chemical transport models; and finally its estimates of the uncertainty in SOA formation yields.
Jing Cai, Kaspar R. Daellenbach, Cheng Wu, Yan Zheng, Feixue Zheng, Wei Du, Sophie L. Haslett, Qi Chen, Markku Kulmala, and Claudia Mohr
Atmos. Meas. Tech., 16, 1147–1165, https://doi.org/10.5194/amt-16-1147-2023, https://doi.org/10.5194/amt-16-1147-2023, 2023
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We introduce the offline application of FIGAERO-CIMS by analyzing Teflon and quartz filter samples that were collected at a typical urban site in Beijing with the deposition time varying from 30 min to 24 h. This method provides a feasible, simple, and quantitative way to investigate the molecular composition and volatility of OA compounds by using FIGAERO-CIMS to analyze offline samples.
William D. Fahy, Cosma Rohilla Shalizi, and Ryan Christopher Sullivan
Atmos. Meas. Tech., 15, 6819–6836, https://doi.org/10.5194/amt-15-6819-2022, https://doi.org/10.5194/amt-15-6819-2022, 2022
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Heterogeneous ice nucleation (IN) alters cloud microphysics and climate, and droplet freezing assays are widely used to determine a material's IN ability. Existing statistical procedures require restrictive assumptions that may bias reported results, and there is no rigorous way to compare IN spectra. To improve the accuracy of reported IN data, we present a method for calculating statistics and confidence bands and testing statistical differences between IN activities in different materials.
Daniela Kau, Marion Greilinger, Bernadette Kirchsteiger, Aron Göndör, Christopher Herzig, Andreas Limbeck, Elisabeth Eitenberger, and Anne Kasper-Giebl
Atmos. Meas. Tech., 15, 5207–5217, https://doi.org/10.5194/amt-15-5207-2022, https://doi.org/10.5194/amt-15-5207-2022, 2022
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The use of thermal–optical analysis for the determination of elemental carbon (EC) and organic carbon (OC) can be biased by mineral dust (MD). We present a method that utilizes this interference to quantify iron contained in MD in snow samples. Possibilities and limitations of applying this method to particulate matter samples are presented. The influence of light-absorbing iron compounds in MD on the transmittance signal can be used to identify samples experiencing a bias of the OC / EC split.
Michael S. Taylor Jr., Devon N. Higgins, and Murray V. Johnston
Atmos. Meas. Tech., 15, 4663–4674, https://doi.org/10.5194/amt-15-4663-2022, https://doi.org/10.5194/amt-15-4663-2022, 2022
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This modelling study investigates the complex growth kinetics of ultrafine particles in a flow tube reactor. When both surface- and volume-limited growth processes occur, the particle diameter growth rate changes as a function of time in the flow tube. We show that this growth can be represented by a parameter (growth factor, GF) which can be obtained experimentally from the outlet-minus-inlet particle diameter change without foreknowledge of the chemical growth processes involved.
Junteng Wu, Nicolas Brun, Juan Miguel González-Sánchez, Badr R'Mili, Brice Temime Roussel, Sylvain Ravier, Jean-Louis Clément, and Anne Monod
Atmos. Meas. Tech., 15, 3859–3874, https://doi.org/10.5194/amt-15-3859-2022, https://doi.org/10.5194/amt-15-3859-2022, 2022
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This work quantified and tentatively identified the organic impurities on ammonium sulfate aerosols generated in the laboratory. They are likely low volatile and high mass molecules containing oxygen, nitrogen, and/or sulfur. Our results show that these organic impurities likely originate from the commercial AS crystals. It is recommended to use AS seeds with caution, especially when small particles are used, in terms of AS purity and water purity when aqueous solutions are used for atomization.
Mohammad R. Sadrian, Wendy M. Calvin, and John McCormack
Atmos. Meas. Tech., 15, 3053–3074, https://doi.org/10.5194/amt-15-3053-2022, https://doi.org/10.5194/amt-15-3053-2022, 2022
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Mineral dust particles originate from surface soils, primarily in arid regions. They can stay suspended in the atmosphere, impacting Earth's radiation budget. Dust particles will have different perturbation effects depending on their composition. We obtained compositional information on dust collected in an urban setting using two different techniques. We recommended using the combination of measurements to determine the variability in dust mineral abundances.
Amir Yazdani, Nikunj Dudani, Satoshi Takahama, Amelie Bertrand, André S. H. Prévôt, Imad El Haddad, and Ann M. Dillner
Atmos. Meas. Tech., 15, 2857–2874, https://doi.org/10.5194/amt-15-2857-2022, https://doi.org/10.5194/amt-15-2857-2022, 2022
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While the aerosol mass spectrometer provides high-time-resolution characterization of the overall extent of oxidation, the extensive fragmentation of molecules and specificity of the technique have posed challenges toward deeper understanding of molecular structures in aerosols. This work demonstrates how functional group information can be extracted from a suite of commonly measured mass fragments using collocated infrared spectroscopy measurements.
Boris Vansevenant, Cédric Louis, Corinne Ferronato, Ludovic Fine, Patrick Tassel, Pascal Perret, Evangelia Kostenidou, Brice Temime-Roussel, Barbara D'Anna, Karine Sartelet, Véronique Cerezo, and Yao Liu
Atmos. Meas. Tech., 14, 7627–7655, https://doi.org/10.5194/amt-14-7627-2021, https://doi.org/10.5194/amt-14-7627-2021, 2021
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A new method was developed to correct wall losses of particles on Teflon walls using a new environmental chamber. It was applied to experiments with six diesel vehicles (Euro 3 to 6), tested on a chassis dynamometer. Emissions of particles and precursors were obtained under urban and motorway conditions. The chamber experiments help understand the role of physical processes in diesel particle evolutions in the dark. These results can be applied to situations such as tunnels or winter rush hours.
Chenyang Bi, Jordan E. Krechmer, Graham O. Frazier, Wen Xu, Andrew T. Lambe, Megan S. Claflin, Brian M. Lerner, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 14, 6835–6850, https://doi.org/10.5194/amt-14-6835-2021, https://doi.org/10.5194/amt-14-6835-2021, 2021
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Iodide-adduct chemical ionization mass spectrometry (I-CIMS) has been widely used to analyze airborne organics. In this study, I-CIMS sensitivities of isomers within a formula are found to generally vary by 1 and up to 2 orders of magnitude. Comparisons between measured and predicted moles, obtained using a voltage-scanning calibration approach, show that predictions for individual compounds or formulas might carry high uncertainty, yet the summed moles of analytes agree reasonably well.
Dimitrios Bousiotis, Ajit Singh, Molly Haugen, David C. S. Beddows, Sebastián Diez, Killian L. Murphy, Pete M. Edwards, Adam Boies, Roy M. Harrison, and Francis D. Pope
Atmos. Meas. Tech., 14, 4139–4155, https://doi.org/10.5194/amt-14-4139-2021, https://doi.org/10.5194/amt-14-4139-2021, 2021
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Measurement and source apportionment of atmospheric pollutants are crucial for the assessment of air quality and the implementation of policies for their improvement. This study highlights the current capability of low-cost sensors in source identification and differentiation using clustering approaches. Future directions towards particulate matter source apportionment using low-cost OPCs are highlighted.
Robert Wagner, Baptiste Testa, Michael Höpfner, Alexei Kiselev, Ottmar Möhler, Harald Saathoff, Jörn Ungermann, and Thomas Leisner
Atmos. Meas. Tech., 14, 1977–1991, https://doi.org/10.5194/amt-14-1977-2021, https://doi.org/10.5194/amt-14-1977-2021, 2021
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During the Asian summer monsoon period, air pollutants are transported from layers near the ground to high altitudes of 13 to 18 km in the atmosphere. Infrared measurements have shown that particles composed of solid ammonium nitrate are a major part of these pollutants. To enable the quantitative analysis of the infrared spectra, we have determined for the first time accurate optical constants of ammonium nitrate for the low-temperature conditions of the upper atmosphere.
David H. Hagan and Jesse H. Kroll
Atmos. Meas. Tech., 13, 6343–6355, https://doi.org/10.5194/amt-13-6343-2020, https://doi.org/10.5194/amt-13-6343-2020, 2020
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Assessing the error of low-cost particulate matter (PM) sensors has been difficult as each empirical study presents unique limitations. Here, we present a new, open-sourced, physics-based model (opcsim) and use it to understand how the properties of different particle sensors alter their accuracy. We offer a summary of likely sources of error for different sensor types, environmental conditions, and particle classes and offer recommendations for the choice of optimal calibrant.
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.
Hanyang Li, Gavin R. McMeeking, and Andrew A. May
Atmos. Meas. Tech., 13, 2865–2886, https://doi.org/10.5194/amt-13-2865-2020, https://doi.org/10.5194/amt-13-2865-2020, 2020
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We present a new correction algorithm that addresses biases in measurements of aerosol light absorption by filter-based photometers, incorporating the transmission of light through the filter and some aerosol optical properties. It was developed using biomass burning aerosols and tested using rural ambient aerosols. This new algorithm is applicable to any filter-based photometer, resulting in good agreement between different colocated instruments in both the laboratory and the field.
Linh Dan Ngo, Dumitru Duca, Yvain Carpentier, Jennifer A. Noble, Raouf Ikhenazene, Marin Vojkovic, Cornelia Irimiea, Ismael K. Ortega, Guillaume Lefevre, Jérôme Yon, Alessandro Faccinetto, Eric Therssen, Michael Ziskind, Bertrand Chazallon, Claire Pirim, and Cristian Focsa
Atmos. Meas. Tech., 13, 951–967, https://doi.org/10.5194/amt-13-951-2020, https://doi.org/10.5194/amt-13-951-2020, 2020
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The partitioning of noxious chemical compounds between the particulate and gas phases in combustion emissions is key to delineate their exact impacts on atmospheric chemistry and human health. We developed a two-filter sampling system, a multi-technique analytical approach, and advanced statistical methods to fully characterize the composition of both phases in combustion emissions. We could successfully discriminate samples from a standard soot generator by their volatile–non-volatile species.
Diep Vu, Shaokai Gao, Tyler Berte, Mary Kacarab, Qi Yao, Kambiz Vafai, and Akua Asa-Awuku
Atmos. Meas. Tech., 12, 4277–4289, https://doi.org/10.5194/amt-12-4277-2019, https://doi.org/10.5194/amt-12-4277-2019, 2019
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Aerosol–cloud interactions contribute the greatest uncertainty to cloud formation. Aerosol composition is complex and can change quickly in the atmosphere. In this work, we recreate a transition in aerosol mixing state in the laboratory, which (to date) has only been observed in the ambient state. We then report the subsequent changes on cloud condensation nuclei (CCN) activation.
Kara D. Lamb
Atmos. Meas. Tech., 12, 3885–3906, https://doi.org/10.5194/amt-12-3885-2019, https://doi.org/10.5194/amt-12-3885-2019, 2019
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Recent atmospheric observations have indicated emissions of iron-oxide-containing aerosols from anthropogenic sources could be 8x higher than previous estimates, leading models to underestimate their climate impact. Previous studies have shown the single particle soot photometer (SP2) can quantify the atmospheric abundance of these aerosols. Here, I explore a machine learning approach to improve SP2 detection, significantly reducing misclassifications of other aerosols as iron oxide aerosols.
Gang Zhao, Weilun Zhao, and Chunsheng Zhao
Atmos. Meas. Tech., 12, 3541–3550, https://doi.org/10.5194/amt-12-3541-2019, https://doi.org/10.5194/amt-12-3541-2019, 2019
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A new method is proposed to retrieve the size-resolved real part of the refractive index (RRI). The main principle of deriving the RRI is measuring the scattering intensity by a single-particle soot photometer of a size-selected aerosol. This method is validated by a series of calibration experiments using the components of the known RI. The retrieved size-resolved RRI covers a wide range, from 200 nm to 450 nm, with uncertainty of less than 0.02.
Matthew Fraund, Tim Park, Lin Yao, Daniel Bonanno, Don Q. Pham, and Ryan C. Moffet
Atmos. Meas. Tech., 12, 1619–1633, https://doi.org/10.5194/amt-12-1619-2019, https://doi.org/10.5194/amt-12-1619-2019, 2019
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Scanning transmission X-ray microscopy (STXM) is a powerful tool which is able to determine the elemental and functional composition of aerosols on a subparticle level. The current work validates the use of STXM for quantitatively calculating the organic volume fraction of individual aerosols by applying the calculation to lab-prepared samples. The caveats and limitations for this calculation are shown as well.
Gabor Vali
Atmos. Meas. Tech., 12, 1219–1231, https://doi.org/10.5194/amt-12-1219-2019, https://doi.org/10.5194/amt-12-1219-2019, 2019
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The abundance of freezing nuclei in water samples is routinely determined by experiments involving the cooling of sample drops and observing the temperatures at which the drops freeze. This is used for characterizing the nucleating abilities of materials in laboratory preparations or to determine the numbers of nucleating particles in rain, snow, river water or other natural waters. The evaluation of drop-freezing experiments in terms of differential nucleus spectra is advocated in the paper.
Ningxin Wang, Spiro D. Jorga, Jeffery R. Pierce, Neil M. Donahue, and Spyros N. Pandis
Atmos. Meas. Tech., 11, 6577–6588, https://doi.org/10.5194/amt-11-6577-2018, https://doi.org/10.5194/amt-11-6577-2018, 2018
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The interaction of particles with the chamber walls has been a significant source of uncertainty when analyzing results of secondary organic aerosol formation experiments performed in Teflon chambers. We evaluated the performance of several particle wall-loss correction methods for aging experiments of α-pinene ozonolysis products. Experimental procedures are proposed for the characterization of particle losses during different stages of these experiments.
Maciej Leśkiewicz, Miron Kaliszewski, Maksymilian Włodarski, Jarosław Młyńczak, Zygmunt Mierczyk, and Krzysztof Kopczyński
Atmos. Meas. Tech., 11, 6259–6270, https://doi.org/10.5194/amt-11-6259-2018, https://doi.org/10.5194/amt-11-6259-2018, 2018
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In this study we demonstrate the application of artificial neural networks to the real-time analysis of single-particle fluorescence fingerprints acquired using BARDet (a BioAeRosol Detector). 48 different aerosols including pollens, bacteria, fungi, spores and nonbiological substances were characterized. An entirely new approach to data analysis using a decision tree comprising 22 independent neural networks was discussed. A very high accuracy of aerosol classification in real time resulted.
Simon Ruske, David O. Topping, Virginia E. Foot, Andrew P. Morse, and Martin W. Gallagher
Atmos. Meas. Tech., 11, 6203–6230, https://doi.org/10.5194/amt-11-6203-2018, https://doi.org/10.5194/amt-11-6203-2018, 2018
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Pollen, bacteria and fungal spores are common in the environment, can have very important implications for public health and may influence the weather. Biological sensors potentially could be used to monitor quantities of these types of particles. However, it is important to transform the measurements from these instruments into counts of these biological particles. The paper tests a variety of approaches for achieving this aim on data collected in a laboratory.
Costa D. Christopoulos, Sarvesh Garimella, Maria A. Zawadowicz, Ottmar Möhler, and Daniel J. Cziczo
Atmos. Meas. Tech., 11, 5687–5699, https://doi.org/10.5194/amt-11-5687-2018, https://doi.org/10.5194/amt-11-5687-2018, 2018
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Compositional analysis of atmospheric and laboratory aerosols is often conducted with mass spectrometry. In this study, machine learning is used to automatically differentiate particles on the basis of chemistry and size. The ability of the machine learning algorithm was then tested on a data set for which the particles were not initially known to judge its ability.
Nicole J. Savage and J. Alex Huffman
Atmos. Meas. Tech., 11, 4929–4942, https://doi.org/10.5194/amt-11-4929-2018, https://doi.org/10.5194/amt-11-4929-2018, 2018
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We show the systematic application of hierarchical agglomerative clustering (HAC) to comprehensive bioaerosol and non-bioaerosol laboratory data collected with the wideband integrated bioaerosol sensor (WIBS-4A). This study investigated various input conditions and used individual matchups and computational mixtures of particles; it will help improve clustering results applied to data from the ultraviolet laser and light-induced fluorescence instruments commonly used for bioaerosol research.
Jake Zenker, Kristen N. Collier, Guanglang Xu, Ping Yang, Ezra J. T. Levin, Kaitlyn J. Suski, Paul J. DeMott, and Sarah D. Brooks
Atmos. Meas. Tech., 10, 4639–4657, https://doi.org/10.5194/amt-10-4639-2017, https://doi.org/10.5194/amt-10-4639-2017, 2017
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We have developed a new method which employs single particle depolarization to determine ice nucleating particle (INP) concentrations and to differentiate between ice crystals, water droplets, and aerosols. The method is used to interpret measurements collected using the Texas A&M Continuous Flow Diffusion Chamber (TAMU CFDC) coupled to a Cloud and Aerosol Spectrometer with Polarization (CASPOL). This new method extends the range of operating conditions for the CFDC to higher supersaturations.
Matthew Osman, Maria A. Zawadowicz, Sarah B. Das, and Daniel J. Cziczo
Atmos. Meas. Tech., 10, 4459–4477, https://doi.org/10.5194/amt-10-4459-2017, https://doi.org/10.5194/amt-10-4459-2017, 2017
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This study presents the first-time attempt at using time-of-flight single particle mass spectrometry (SPMS) as an emerging online technique for measuring insoluble particles in glacial snow and ice. Using samples from two Greenlandic ice cores, we show that SPMS can constrain the aerodynamic size, composition, and relative abundance of most particulate types on a per-particle basis, reducing the preparation time and resources required of conventional, filter-based particle retrieval methods.
Simon Ruske, David O. Topping, Virginia E. Foot, Paul H. Kaye, Warren R. Stanley, Ian Crawford, Andrew P. Morse, and Martin W. Gallagher
Atmos. Meas. Tech., 10, 695–708, https://doi.org/10.5194/amt-10-695-2017, https://doi.org/10.5194/amt-10-695-2017, 2017
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Particles such as bacteria, pollen and fungal spores have important implications within the environment and public health sectors. Here we evaluate the performance of various different methods for distinguishing between these different types of particles using a new instrument. We demonstrate that there may be better alternatives to the currently used methods which can be further investigated in future research.
Yan Lyu, Tingting Xu, Xiang Li, Tiantao Cheng, Xin Yang, Xiaomin Sun, and Jianmin Chen
Atmos. Meas. Tech., 9, 1025–1037, https://doi.org/10.5194/amt-9-1025-2016, https://doi.org/10.5194/amt-9-1025-2016, 2016
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This study presents the particle size distribution of PBDEs in the atmosphere of a megacity and evaluates the contribution of size-fractionated PBDEs' deposition in the human respiratory tract.
Matteo Reggente, Ann M. Dillner, and Satoshi Takahama
Atmos. Meas. Tech., 9, 441–454, https://doi.org/10.5194/amt-9-441-2016, https://doi.org/10.5194/amt-9-441-2016, 2016
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Organic carbon and elemental carbon are major components of atmospheric PM. Typically they are measured using destructive and relatively expensive methods (e.g., TOR). We aim to reduce the operating costs of large air quality monitoring networks using FT-IR spectra of ambient PTFE filters and PLS regression. We achieve accurate predictions for models (calibrated in 2011) that use samples collected at the same or different sites of the calibration data set and in a different year (2013).
S. S. Steimer, U. K. Krieger, Y.-F. Te, D. M. Lienhard, A. J. Huisman, B. P. Luo, M. Ammann, and T. Peter
Atmos. Meas. Tech., 8, 2397–2408, https://doi.org/10.5194/amt-8-2397-2015, https://doi.org/10.5194/amt-8-2397-2015, 2015
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Atmospheric aerosol is often subject to supersaturated or supercooled conditions where bulk measurements are not possible. Here we demonstrate how measurements using single particle electrodynamic levitation combined with light scattering spectroscopy allow the retrieval of thermodynamic data, optical properties and water diffusivity of such metastable particles even when auxiliary bulk data are not available due to lack of sufficient amounts of sample.
N. Utry, T. Ajtai, M. Pintér, E. Tombácz, E. Illés, Z. Bozóki, and G. Szabó
Atmos. Meas. Tech., 8, 401–410, https://doi.org/10.5194/amt-8-401-2015, https://doi.org/10.5194/amt-8-401-2015, 2015
A. Quérel, P. Lemaitre, M. Monier, E. Porcheron, A. I. Flossmann, and M. Hervo
Atmos. Meas. Tech., 7, 1321–1330, https://doi.org/10.5194/amt-7-1321-2014, https://doi.org/10.5194/amt-7-1321-2014, 2014
F. Freutel, F. Drewnick, J. Schneider, T. Klimach, and S. Borrmann
Atmos. Meas. Tech., 6, 3131–3145, https://doi.org/10.5194/amt-6-3131-2013, https://doi.org/10.5194/amt-6-3131-2013, 2013
E. Fuentes and G. McFiggans
Atmos. Meas. Tech., 5, 735–757, https://doi.org/10.5194/amt-5-735-2012, https://doi.org/10.5194/amt-5-735-2012, 2012
C. D. Cappa
Atmos. Meas. Tech., 3, 579–592, https://doi.org/10.5194/amt-3-579-2010, https://doi.org/10.5194/amt-3-579-2010, 2010
Cited articles
Al-Naiema, I. M., Offenberg, J. H., Madler, C. J., Lewandowski, M., Kettler,
J., Fang, T., and Stone, E. A.: Secondary Organic Aerosols from Aromatic
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Brüggemann, M., Xu, R., Tilgner, A., Kwong, K. C., Mutzel, A., Poon, H. Y.,
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Keutsch, F. N., Kroll, J. H., McNeill, V. F., Ng, N. L., Nizkorodov, S. A.,
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Chen, X., Xie, M., Hays, M. D., Edgerton, E., Schwede, D., and Walker, J. T.: Characterization of organic nitrogen in aerosols at a forest site in the southern Appalachian Mountains, Atmos. Chem. Phys., 18, 6829–6846, https://doi.org/10.5194/acp-18-6829-2018, 2018. a, b
Chen, Y., Takeuchi, M., Nah, T., Xu, L., Canagaratna, M. R., Stark, H., Baumann, K., Canonaco, F., Prévôt, A. S. H., Huey, L. G., Weber, R. J., and Ng, N. L.: Chemical characterization of secondary organic aerosol at a rural site in the southeastern US: insights from simultaneous high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and FIGAERO chemical ionization mass spectrometer (CIMS) measurements, Atmos. Chem. Phys., 20, 8421–8440, https://doi.org/10.5194/acp-20-8421-2020, 2020. a
Christoffersen, T., Hjorth, J., Horie, O., Jensen, N., Kotzias, D., Molander,
L., Neeb, P., Ruppert, L., Winterhalter, R., Virkkula, A., Wirtz, K., and
Larsen, B.: cis-pinic acid, a possible precursor for organic aerosol
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Claeys, M. and Maenhaut, W.: Secondary Organic Aerosol Formation from Isoprene:
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Claeys, M., Iinuma, Y., Szmigielski, R., Surratt, J. D., Blockhuys, F.,
Van Alsenoy, C., Böge, O., Sierau, B., Gómez-González, Y., Vermeylen, R.,
Van der Veken, P., Shahgholi, M., Chan, A. W. H., Herrmann, H., Seinfeld,
J. H., and Maenhaut, W.: Terpenylic Acid and Related Compounds from the
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Daellenbach, K. R., Kourtchev, I., Vogel, A. L., Bruns, E. A., Jiang, J., Petäjä, T., Jaffrezo, J.-L., Aksoyoglu, S., Kalberer, M., Baltensperger, U., El Haddad, I., and Prévôt, A. S. H.: Impact of anthropogenic and biogenic sources on the seasonal variation in the molecular composition of urban organic aerosols: a field and laboratory study using ultra-high-resolution mass spectrometry, Atmos. Chem. Phys., 19, 5973–5991, https://doi.org/10.5194/acp-19-5973-2019, 2019. a
Ditto, J. C., Barnes, E. B., Khare, P., Takeuchi, M., Joo, T., Bui, A. A. T.,
Lee-Taylor, J., Eris, G., Chen, Y., Aumont, B., Jimenez, J. L., Ng, N. L.,
Griffin, R. J., and Gentner, D. R.: An omnipresent diversity and variability
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Gao, Y., Hall, W. A., and Johnston, M. V.: Molecular Composition of Monoterpene
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Short summary
We introduce the aerosolomics database and apply it to particulate matter samples. Nine VOCs were oxidized under various conditions in an oxidation flow reactor, and the formed SOA was measured using liquid chromatography mass spectrometry. With the database, an unambiguous top-down attribution of atmospheric oxidation products to their parent VOCs is now possible. Combining the database with hierarchical clustering enables a better understanding of sources, formation, and partitioning of SOA.
We introduce the aerosolomics database and apply it to particulate matter samples. Nine VOCs...
