Articles | Volume 12, issue 12
https://doi.org/10.5194/amt-12-6635-2019
© Author(s) 2019. 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-12-6635-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
17 Dec 2019
Research article |
| 17 Dec 2019
| 17 Dec 2019
Multi-scheme chemical ionization inlet (MION) for fast switching of reagent ion chemistry in atmospheric pressure chemical ionization mass spectrometry (CIMS) applications
Department of Physics and Institute for Atmospheric and Earth System
Research, University of Helsinki, Helsinki, Finland
Aerosol Physics Laboratory, Physics Unit, Faculty of Engineering and
Natural Sciences, Tampere University, Tampere, Finland
Jyri Mikkilä
Karsa Ltd., A. I. Virtasen aukio 1, 00560 Helsinki, Finland
Siddharth Iyer
Aerosol Physics Laboratory, Physics Unit, Faculty of Engineering and
Natural Sciences, Tampere University, Tampere, Finland
Department of Chemistry and Institute for Atmospheric and Earth System
Research, University of Helsinki, Helsinki, Finland
Jani Hakala
CORRESPONDING AUTHOR
Karsa Ltd., A. I. Virtasen aukio 1, 00560 Helsinki, Finland
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Secondary organic aerosols (SOA) form effectively from gaseous precursors via a process called autoxidation. While key chemical reaction types seem to be known, no general description of autoxidation chemistry exists. In the present work, we present a method to create autoxidation chemistry schemes for any atmospherically relevant hydrocarbon. We exemplarily investigate benzene and its potential to form aerosols. We found that autoxidation, under some conditions, can dominate the SOA formation.
Melissa Meder, Otso Peräkylä, Jonathan G. Varelas, Jingyi Luo, Runlong Cai, Yanjun Zhang, Theo Kurtén, Matthieu Riva, Matti Rissanen, Franz M. Geiger, Regan J. Thomson, and Mikael Ehn
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Miska Olin, Magdalena Okuljar, Matti P. Rissanen, Joni Kalliokoski, Jiali Shen, Lubna Dada, Markus Lampimäki, Yusheng Wu, Annalea Lohila, Jonathan Duplissy, Mikko Sipilä, Tuukka Petäjä, Markku Kulmala, and Miikka Dal Maso
Atmos. Chem. Phys., 22, 8097–8115, https://doi.org/10.5194/acp-22-8097-2022, https://doi.org/10.5194/acp-22-8097-2022, 2022
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Atmospheric new particle formation is an important source of the total particle number concentration in the atmosphere. Several parameters for predicting new particle formation events have been suggested before, but the results have been inconclusive. This study proposes an another predicting parameter, related to a specific type of highly oxidized organic molecules, especially for similar locations to the measurement site in this study, which was a coastal agricultural site in Finland.
Dalrin Ampritta Amaladhasan, Claudia Heyn, Christopher R. Hoyle, Imad El Haddad, Miriam Elser, Simone M. Pieber, Jay G. Slowik, Antonio Amorim, Jonathan Duplissy, Sebastian Ehrhart, Vladimir Makhmutov, Ugo Molteni, Matti Rissanen, Yuri Stozhkov, Robert Wagner, Armin Hansel, Jasper Kirkby, Neil M. Donahue, Rainer Volkamer, Urs Baltensperger, Martin Gysel-Beer, and Andreas Zuend
Atmos. Chem. Phys., 22, 215–244, https://doi.org/10.5194/acp-22-215-2022, https://doi.org/10.5194/acp-22-215-2022, 2022
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Mingyi Wang, Xu-Cheng He, Henning Finkenzeller, Siddharth Iyer, Dexian Chen, Jiali Shen, Mario Simon, Victoria Hofbauer, Jasper Kirkby, Joachim Curtius, Norbert Maier, Theo Kurtén, Douglas R. Worsnop, Markku Kulmala, Matti Rissanen, Rainer Volkamer, Yee Jun Tham, Neil M. Donahue, and Mikko Sipilä
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Meri Räty, Otso Peräkylä, Matthieu Riva, Lauriane Quéléver, Olga Garmash, Matti Rissanen, and Mikael Ehn
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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.
Clémence Rose, Matti P. Rissanen, Siddharth Iyer, Jonathan Duplissy, Chao Yan, John B. Nowak, Aurélie Colomb, Régis Dupuy, Xu-Cheng He, Janne Lampilahti, Yee Jun Tham, Daniela Wimmer, Jean-Marc Metzger, Pierre Tulet, Jérôme Brioude, Céline Planche, Markku Kulmala, and Karine Sellegri
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Sulfuric acid (H2SO4) is commonly accepted as a key precursor for atmospheric new particle formation. However, direct measurements of [H2SO4] remain challenging, motivating the development of proxies. Using data collected in two different volcanic plumes, we show, under these specific conditions, the good performance of a proxy from the literature and also highlight the benefit of the newly developed proxies for the prediction of the highest [H2SO4] values.
Martin Heinritzi, Lubna Dada, Mario Simon, Dominik Stolzenburg, Andrea C. Wagner, Lukas Fischer, Lauri R. Ahonen, Stavros Amanatidis, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Bernhard Baumgartner, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, Antonio Dias, Josef Dommen, Jonathan Duplissy, Henning Finkenzeller, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Manuel Granzin, Imad El Haddad, Xucheng He, Johanna Helm, Victoria Hofbauer, Christopher R. Hoyle, Juha Kangasluoma, Timo Keber, Changhyuk Kim, Andreas Kürten, Houssni Lamkaddam, Tiia M. Laurila, Janne Lampilahti, Chuan Ping Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Vladimir Makhmutov, Hanna Elina Manninen, Ruby Marten, Serge Mathot, Roy Lee Mauldin, Bernhard Mentler, Ugo Molteni, Tatjana Müller, Wei Nie, Tuomo Nieminen, Antti Onnela, Eva Partoll, Monica Passananti, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti P. Rissanen, Clémence Rose, Siegfried Schobesberger, Wiebke Scholz, Kay Scholze, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, Miguel Vazquez-Pufleau, Annele Virtanen, Alexander L. Vogel, Rainer Volkamer, Robert Wagner, Mingyi Wang, Lena Weitz, Daniela Wimmer, Mao Xiao, Chao Yan, Penglin Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Urs Baltensperger, Armin Hansel, Markku Kulmala, António Tomé, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 11809–11821, https://doi.org/10.5194/acp-20-11809-2020, https://doi.org/10.5194/acp-20-11809-2020, 2020
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With experiments performed at CLOUD, we show how isoprene interferes in monoterpene oxidation via RO2 termination at atmospherically relevant concentrations. This interference shifts the distribution of highly oxygenated organic molecules (HOMs) away from C20 class dimers towards C15 class dimers, which subsequently reduces both biogenic nucleation and early growth rates. Our results may help to understand the absence of new-particle formation in isoprene-rich environments.
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.
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.
Dean Chen, Putian Zhou, Tuomo Nieminen, Pontus Roldin, Ximeng Qi, Petri Clusius, Carlton Xavier, Lukas Pichelstorfer, Markku Kulmala, Pekka Rantala, Juho Aalto, Nina Sarnela, Pasi Kolari, Petri Keronen, Matti P. Rissanen, Metin Baykara, and Michael Boy
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-128, https://doi.org/10.5194/acp-2020-128, 2020
Preprint withdrawn
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Atmospheric oxidants OH, O3 and NO3 dominate the atmospheric oxidation capacity, and sulfuric acid (H2SO4) is considered as a main driver for new particle formation events. We studied how the trends of these atmospheric oxidants and H2SO4 changed in southern Finland during the past 12 years and discussed how these trends related to decreasing emissions of air pollutants in Europe. Our results showed that OH increased by 1.56 % yr−1 at daytime and NO3 decreased by 3.92 % yr−1 at nighttime.
Olga Garmash, Matti P. Rissanen, Iida Pullinen, Sebastian Schmitt, Oskari Kausiala, Ralf Tillmann, Defeng Zhao, Carl Percival, Thomas J. Bannan, Michael Priestley, Åsa M. Hallquist, Einhard Kleist, Astrid Kiendler-Scharr, Mattias Hallquist, Torsten Berndt, Gordon McFiggans, Jürgen Wildt, Thomas F. Mentel, and Mikael Ehn
Atmos. Chem. Phys., 20, 515–537, https://doi.org/10.5194/acp-20-515-2020, https://doi.org/10.5194/acp-20-515-2020, 2020
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Highly oxygenated organic molecules (HOMs) facilitate aerosol formation in the atmosphere. Using NO3− chemical ionization mass spectrometry we investigated HOM composition and yield in oxidation of aromatic compounds at different reactant concentrations, in the presence of NOx and seed aerosol. Higher OH concentrations increased HOM yield, suggesting multiple oxidation steps, and affected HOM composition, potentially explaining in part discrepancies in published secondary organic aerosol yields.
Ximeng Qi, Aijun Ding, Pontus Roldin, Zhengning Xu, Putian Zhou, Nina Sarnela, Wei Nie, Xin Huang, Anton Rusanen, Mikael Ehn, Matti P. Rissanen, Tuukka Petäjä, Markku Kulmala, and Michael Boy
Atmos. Chem. Phys., 18, 11779–11791, https://doi.org/10.5194/acp-18-11779-2018, https://doi.org/10.5194/acp-18-11779-2018, 2018
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In this study we simulate the HOM concentrations and discuss their roles in NPF at a remote boreal forest site in Finland and a suburban site in eastern China. We found that sulfuric acid and HOM organonitrate concentrations in the gas phase are significantly higher but other HOM monomers and dimers from monoterpene oxidation are lower in eastern China. This study highlights the need for molecular-scale measurements in improving the understanding of NPF mechanisms in polluted areas.
Nina Sarnela, Tuija Jokinen, Jonathan Duplissy, Chao Yan, Tuomo Nieminen, Mikael Ehn, Siegfried Schobesberger, Martin Heinritzi, Sebastian Ehrhart, Katrianne Lehtipalo, Jasmin Tröstl, Mario Simon, Andreas Kürten, Markus Leiminger, Michael J. Lawler, Matti P. Rissanen, Federico Bianchi, Arnaud P. Praplan, Jani Hakala, Antonio Amorim, Marc Gonin, Armin Hansel, Jasper Kirkby, Josef Dommen, Joachim Curtius, James N. Smith, Tuukka Petäjä, Douglas R. Worsnop, Markku Kulmala, Neil M. Donahue, and Mikko Sipilä
Atmos. Chem. Phys., 18, 2363–2380, https://doi.org/10.5194/acp-18-2363-2018, https://doi.org/10.5194/acp-18-2363-2018, 2018
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Atmospheric trace gases can form small molecular clusters, which can grow to larger sizes through the condensation of vapours. This process is called new particle formation. In this paper we studied the formation of sulfuric acid and highly oxygenated molecules, the key compounds in atmospheric new particle formation, in chamber experiments and introduced a way to simulate these ozonolysis products of α-pinene in a simple manner.
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.
Xuemeng Chen, Lauriane L. J. Quéléver, Pak L. Fung, Jutta Kesti, Matti P. Rissanen, Jaana Bäck, Petri Keronen, Heikki Junninen, Tuukka Petäjä, Veli-Matti Kerminen, and Markku Kulmala
Atmos. Chem. Phys., 18, 49–63, https://doi.org/10.5194/acp-18-49-2018, https://doi.org/10.5194/acp-18-49-2018, 2018
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We analysed a 20-year-long dataset collected in a Finnish boreal forest at SMEAR II station to investigate the frequency and strength of ozone depletion events. We could identify a number of ozone depletion events that lasted for more than 3 h, mainly in the autumn and winter months. Their occurrence was likely related to the formation of a low mixing layer under the conditions of low temperatures, low wind speeds, high relative humidities and limited intensity of solar radiation.
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
Putian Zhou, Laurens Ganzeveld, Ditte Taipale, Üllar Rannik, Pekka Rantala, Matti Petteri Rissanen, Dean Chen, and Michael Boy
Atmos. Chem. Phys., 17, 14309–14332, https://doi.org/10.5194/acp-17-14309-2017, https://doi.org/10.5194/acp-17-14309-2017, 2017
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In boreal forest, there is a large number of gaseous organic compounds called biogenic volatile organic compounds (BVOCs). Within the canopy, they can be emitted from vegetation and soil, react with each other and other gases, be transported in the air, and be removed from vegetation and soil surfaces. We applied a numerical model to simulate these processes and found that these BVOCs can be divided into five categories according to the significance of their sources and sinks.
Federico Bianchi, Olga Garmash, Xucheng He, Chao Yan, Siddharth Iyer, Ida Rosendahl, Zhengning Xu, Matti P. Rissanen, Matthieu Riva, Risto Taipale, Nina Sarnela, Tuukka Petäjä, Douglas R. Worsnop, Markku Kulmala, Mikael Ehn, and Heikki Junninen
Atmos. Chem. Phys., 17, 13819–13831, https://doi.org/10.5194/acp-17-13819-2017, https://doi.org/10.5194/acp-17-13819-2017, 2017
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Naturally charged highly oxidised molecules (HOMs) were characterized using advanced mass spectrometers. Two different classes of compounds, clustered with the nitrate and bisulfate ions, were identified: HOMs containing only carbon, hydrogen and oxygen and nitrogen-containing HOMs or organonitrates (ONs). They exhibit strong diurnal variations where HOMs peak during night and ONs during day. Finally, large clusters containing up to 40 carbon atoms (four oxidized
α-pinene units) were observed.
Emilie Öström, Zhou Putian, Guy Schurgers, Mikhail Mishurov, Niku Kivekäs, Heikki Lihavainen, Mikael Ehn, Matti P. Rissanen, Theo Kurtén, Michael Boy, Erik Swietlicki, and Pontus Roldin
Atmos. Chem. Phys., 17, 8887–8901, https://doi.org/10.5194/acp-17-8887-2017, https://doi.org/10.5194/acp-17-8887-2017, 2017
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We used a model to study how biogenic volatile organic compounds (BVOCs) emitted from the boreal forest contribute to the formation and growth of particles in the atmosphere. Some of these particles are important climate forcers, acting as seeds for cloud droplet fomation. We implemented a new gas chemistry mechanism that describes how the BVOCs are oxidized and form low-volatility highly oxidized organic molecules. With the new mechanism we are able to accurately predict the particle growth.
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.
Chao Yan, Wei Nie, Mikko Äijälä, Matti P. Rissanen, Manjula R. Canagaratna, Paola Massoli, Heikki Junninen, Tuija Jokinen, Nina Sarnela, Silja A. K. Häme, Siegfried Schobesberger, Francesco Canonaco, Lei Yao, André S. H. Prévôt, Tuukka Petäjä, Markku Kulmala, Mikko Sipilä, Douglas R. Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 16, 12715–12731, https://doi.org/10.5194/acp-16-12715-2016, https://doi.org/10.5194/acp-16-12715-2016, 2016
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Highly oxidized multifunctional compounds (HOMs) are known to have a significant contribution to secondary aerosol formation, yet their dominating formation pathways remain unclear in the atmosphere. We apply positive matrix factorization (PMF) on HOM data, and successfully retrieve factors representing different formation pathways. The results improve our understanding of HOM formation, and provide new perspectives on using PMF to study the variation of short-lived specie.
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.
R. L. Mauldin III, M. P. Rissanen, T. Petäjä, and M. Kulmala
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2015-398, https://doi.org/10.5194/amt-2015-398, 2016
Revised manuscript not accepted
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The manuscript describes a novel instrument for the measurement of OH, HO2+RO2, and other atmospheric species. The instrument described combines the chemical ionization techniques of nitrate CIMS, OH conversion to H2SO4, HO2+RO2 conversion to H2SO4, and high resolution time of flight mass spectroscopy into one system. By using one instrument to obtain spectra it is possible to compare spectra from the different modes and gain further chemical information towards peak identification.
M. Sipilä, N. Sarnela, T. Jokinen, H. Junninen, J. Hakala, M. P. Rissanen, A. Praplan, M. Simon, A. Kürten, F. Bianchi, J. Dommen, J. Curtius, T. Petäjä, and D. R. Worsnop
Atmos. Meas. Tech., 8, 4001–4011, https://doi.org/10.5194/amt-8-4001-2015, https://doi.org/10.5194/amt-8-4001-2015, 2015
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Atmospheric concentrations of amines are poorly known mainly due to challenges related to their reliable high-sensitivity detection. We have created a method and instrument that is capable for detecting amines with lowest limit of detection of around 0.01 parts per trillion. Application of the instrument in the field study indicates that concentrations of dimethyl amine in a boreal forest site are below 0.03ppt, not enough to account for the observed new particle formation rates.
T. F. Mentel, M. Springer, M. Ehn, E. Kleist, I. Pullinen, T. Kurtén, M. Rissanen, A. Wahner, and J. Wildt
Atmos. Chem. Phys., 15, 6745–6765, https://doi.org/10.5194/acp-15-6745-2015, https://doi.org/10.5194/acp-15-6745-2015, 2015
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We studied a series of cycloalkenes and methyl-substituted alkenes in order to elucidate the structural pre-requisites and chemical pathways to the recently discovered class of highly oxidized molecules ELVOC (Ehn et al., Nature, 2014). ELVOC may totally change the view on (parts of) the mechanism of SOA formation. We present results which support recent observations of H shifts from C-H to peroxy radicals, highlighting the pivotal role of peroxyradicals in organic atmospheric chemistry.
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.
M. Sipilä, T. Jokinen, T. Berndt, S. Richters, R. Makkonen, N. M. Donahue, R. L. Mauldin III, T. Kurtén, P. Paasonen, N. Sarnela, M. Ehn, H. Junninen, M. P. Rissanen, J. Thornton, F. Stratmann, H. Herrmann, D. R. Worsnop, M. Kulmala, V.-M. Kerminen, and T. Petäjä
Atmos. Chem. Phys., 14, 12143–12153, https://doi.org/10.5194/acp-14-12143-2014, https://doi.org/10.5194/acp-14-12143-2014, 2014
J. Kangasluoma, C. Kuang, D. Wimmer, M. P. Rissanen, K. Lehtipalo, M. Ehn, D. R. Worsnop, J. Wang, M. Kulmala, and T. Petäjä
Atmos. Meas. Tech., 7, 689–700, https://doi.org/10.5194/amt-7-689-2014, https://doi.org/10.5194/amt-7-689-2014, 2014
Henning Finkenzeller, Jyri Mikkilä, Cecilia Righi, Paxton Juuti, Mikko Sipilä, Matti Rissanen, Douglas Worsnop, Aleksei Shcherbinin, Nina Sarnela, and Juha Kangasluoma
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2024-48, https://doi.org/10.5194/amt-2024-48, 2024
Preprint under review for AMT
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Chemical ionization mass spectrometry is used in atmospheric sciences to measure trace gas concentrations. Neutral gases require charging in inlets before the mass-to-charge ratio of the resulting ions can be analyzed. This study uses multi-physics modelling to investigate how the MION2 and Eisele type inlets work, shows the effect of tuning parameters, and their current limitations. The findings are helpful for the inlet users and are expected to aid in developing improved inlets.
Alex Rowell, James Brean, David C. S. Beddows, Zongbo Shi, Avinash Kumar, Matti Rissanen, Miikka Dal Maso, Peter Mettke, Kay Weinhold, Maik Merkel, and Roy M. Harrison
EGUsphere, https://doi.org/10.5194/egusphere-2024-742, https://doi.org/10.5194/egusphere-2024-742, 2024
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Ions enhance the formation and growth rates of new particles, affecting the earths radiation budget. Despite these effects, there is little published data exploring the sources of ions in the urban environment and their role in new particle formation (NPF). Here we show that natural ion sources dominate in urban environments, while traffic is a secondary source. Ions contribute up to 12.7 % of the formation rate of particles, indicating that they are important for forming urban PM.
Romain Salignat, Matti Rissanen, Siddharth Iyer, Jean-Luc Baray, Pierre Tulet, Jean-Marc Metzger, Jérôme Brioude, Karine Sellegri, and Clémence Rose
Atmos. Chem. Phys., 24, 3785–3812, https://doi.org/10.5194/acp-24-3785-2024, https://doi.org/10.5194/acp-24-3785-2024, 2024
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Using mass spectrometry data collected at the Maïdo Observatory (2160 m a.s.l., Réunion), we provide the first detailed analysis of molecular cluster chemical composition specifically in the marine free troposphere. The abundance of the identified species is related both to in situ meteorological parameters and air mass history, which also provide insight into their origin. Our work makes an important contribution to documenting the chemistry and physics of the marine free troposphere.
Stéphanie Alage, Vincent Michoud, Sergio Harb, Bénédicte Picquet-Varrault, Manuela Cirtog, Avinash Kumar, Matti Rissanen, and Christopher Cantrell
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2024-20, https://doi.org/10.5194/amt-2024-20, 2024
Revised manuscript accepted for AMT
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Calibration exercises are essential for determining the accuracy of instruments. We performed calibrations on a NO3¯ ToFCIMS instrument to determine its sensitivity and linearity for detecting various organic compounds. Our findings revealed significant variability, over several orders of magnitude, in the calibration factors obtained. The results suggest that relying on a single calibration factor from H2SO4 for the quantification of all compounds detected by this technique is not appropriate.
Xu-Cheng He, Jiali Shen, Siddharth Iyer, Paxton Juuti, Jiangyi Zhang, Mrisha Koirala, Mikko M. Kytökari, Douglas R. Worsnop, Matti Rissanen, Markku Kulmala, Norbert M. Maier, Jyri Mikkilä, Mikko Sipilä, and Juha Kangasluoma
Atmos. Meas. Tech., 16, 4461–4487, https://doi.org/10.5194/amt-16-4461-2023, https://doi.org/10.5194/amt-16-4461-2023, 2023
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In this study, the upgraded multi-scheme chemical ionisation inlet 2 is presented. Sulfuric acid, hypoiodous acid, iodine, sulfur dioxide, and hydroperoxyl radicals are calibrated, and the improved ion optics allow us to detect sulfuric acid and iodine-containing molecules at as low as a few parts per quadrillion by volume. Additionally, we confirm the reliable detection of iodic acid using both the nitrate and bromide chemical ionisation methods under atmospherically relevant conditions.
Shawon Barua, Siddharth Iyer, Avinash Kumar, Prasenjit Seal, and Matti Rissanen
Atmos. Chem. Phys., 23, 10517–10532, https://doi.org/10.5194/acp-23-10517-2023, https://doi.org/10.5194/acp-23-10517-2023, 2023
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This work illustrates how a common volatile hydrocarbon, hexanal, has the potential to undergo atmospheric autoxidation that leads to prompt formation of condensable material that subsequently contributes to aerosol formation, deteriorating the air quality of urban atmospheres. We used the combined state-of-the-art quantum chemical modeling and experimental flow reactor experiments under atmospheric conditions to resolve the autoxidation mechanism of hexanal initiated by a common oxidant.
Lukas Pichelstorfer, Pontus Roldin, Matti Rissanen, Noora Hyttinen, Olga Garmash, Carlton Xavier, Putian Zhou, Petri Clusius, Benjamin Foreback, Thomas Golin Almeida, Chenjuan Deng, Metin Baykara, Theo Kurten, and Michael Boy
EGUsphere, https://doi.org/10.5194/egusphere-2023-1415, https://doi.org/10.5194/egusphere-2023-1415, 2023
Preprint archived
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Secondary organic aerosols (SOA) form effectively from gaseous precursors via a process called autoxidation. While key chemical reaction types seem to be known, no general description of autoxidation chemistry exists. In the present work, we present a method to create autoxidation chemistry schemes for any atmospherically relevant hydrocarbon. We exemplarily investigate benzene and its potential to form aerosols. We found that autoxidation, under some conditions, can dominate the SOA formation.
Melissa Meder, Otso Peräkylä, Jonathan G. Varelas, Jingyi Luo, Runlong Cai, Yanjun Zhang, Theo Kurtén, Matthieu Riva, Matti Rissanen, Franz M. Geiger, Regan J. Thomson, and Mikael Ehn
Atmos. Chem. Phys., 23, 4373–4390, https://doi.org/10.5194/acp-23-4373-2023, https://doi.org/10.5194/acp-23-4373-2023, 2023
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We discuss and show the viability of a method where multiple isotopically labelled precursors are used for probing the formation pathways of highly oxygenated organic molecules (HOMs) from the oxidation of the monoterpene a-pinene. HOMs are very important for secondary organic aerosol (SOA) formation in forested regions, and monoterpenes are the single largest source of SOA globally. The fast reactions forming HOMs have thus far remained elusive despite considerable efforts over the last decade.
Miska Olin, Magdalena Okuljar, Matti P. Rissanen, Joni Kalliokoski, Jiali Shen, Lubna Dada, Markus Lampimäki, Yusheng Wu, Annalea Lohila, Jonathan Duplissy, Mikko Sipilä, Tuukka Petäjä, Markku Kulmala, and Miikka Dal Maso
Atmos. Chem. Phys., 22, 8097–8115, https://doi.org/10.5194/acp-22-8097-2022, https://doi.org/10.5194/acp-22-8097-2022, 2022
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Atmospheric new particle formation is an important source of the total particle number concentration in the atmosphere. Several parameters for predicting new particle formation events have been suggested before, but the results have been inconclusive. This study proposes an another predicting parameter, related to a specific type of highly oxidized organic molecules, especially for similar locations to the measurement site in this study, which was a coastal agricultural site in Finland.
Dalrin Ampritta Amaladhasan, Claudia Heyn, Christopher R. Hoyle, Imad El Haddad, Miriam Elser, Simone M. Pieber, Jay G. Slowik, Antonio Amorim, Jonathan Duplissy, Sebastian Ehrhart, Vladimir Makhmutov, Ugo Molteni, Matti Rissanen, Yuri Stozhkov, Robert Wagner, Armin Hansel, Jasper Kirkby, Neil M. Donahue, Rainer Volkamer, Urs Baltensperger, Martin Gysel-Beer, and Andreas Zuend
Atmos. Chem. Phys., 22, 215–244, https://doi.org/10.5194/acp-22-215-2022, https://doi.org/10.5194/acp-22-215-2022, 2022
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We use a combination of models for gas-phase chemical reactions and equilibrium gas–particle partitioning of isoprene-derived secondary organic aerosols (SOAs) informed by dark ozonolysis experiments conducted in the CLOUD chamber. Our predictions cover high to low relative humidities (RHs) and quantify how SOA mass yields are enhanced at high RH as well as the impact of inorganic seeds of distinct hygroscopicities and acidities on the coupled partitioning of water and semi-volatile organics.
Mao Xiao, Christopher R. Hoyle, Lubna Dada, Dominik Stolzenburg, Andreas Kürten, Mingyi Wang, Houssni Lamkaddam, Olga Garmash, Bernhard Mentler, Ugo Molteni, Andrea Baccarini, Mario Simon, Xu-Cheng He, Katrianne Lehtipalo, Lauri R. Ahonen, Rima Baalbaki, Paulus S. Bauer, Lisa Beck, David Bell, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, António Dias, Jonathan Duplissy, Henning Finkenzeller, Hamish Gordon, Victoria Hofbauer, Changhyuk Kim, Theodore K. Koenig, Janne Lampilahti, Chuan Ping Lee, Zijun Li, Huajun Mai, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Serge Mathot, Roy L. Mauldin, Wei Nie, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti Rissanen, Siegfried Schobesberger, Simone Schuchmann, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Robert Wagner, Yonghong Wang, Lena Weitz, Daniela Wimmer, Yusheng Wu, Chao Yan, Penglin Ye, Qing Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Ken Carslaw, Joachim Curtius, Armin Hansel, Rainer Volkamer, Paul M. Winkler, Richard C. Flagan, Markku Kulmala, Douglas R. Worsnop, Jasper Kirkby, Neil M. Donahue, Urs Baltensperger, Imad El Haddad, and Josef Dommen
Atmos. Chem. Phys., 21, 14275–14291, https://doi.org/10.5194/acp-21-14275-2021, https://doi.org/10.5194/acp-21-14275-2021, 2021
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Experiments at CLOUD show that in polluted environments new particle formation (NPF) is largely driven by the formation of sulfuric acid–base clusters, stabilized by amines, high ammonia concentrations or lower temperatures. While oxidation products of aromatics can nucleate, they play a minor role in urban NPF. Our experiments span 4 orders of magnitude variation of observed NPF rates in ambient conditions. We provide a framework based on NPF and growth rates to interpret ambient observations.
Wei Huang, Haiyan Li, Nina Sarnela, Liine Heikkinen, Yee Jun Tham, Jyri Mikkilä, Steven J. Thomas, Neil M. Donahue, Markku Kulmala, and Federico Bianchi
Atmos. Chem. Phys., 21, 8961–8977, https://doi.org/10.5194/acp-21-8961-2021, https://doi.org/10.5194/acp-21-8961-2021, 2021
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We show full characterization of gaseous organic compounds in a boreal forest. Molecular composition and volatility of gaseous organic compounds with different oxidation extents (from volatile organic compounds to highly oxygenated organic molecules) were investigated and discussed. We provide a more comprehensive understanding of atmospheric organic compounds in this boreal forest and new insights into interpreting ambient measurements or testing and improving parameterizations in models.
Mingyi Wang, Xu-Cheng He, Henning Finkenzeller, Siddharth Iyer, Dexian Chen, Jiali Shen, Mario Simon, Victoria Hofbauer, Jasper Kirkby, Joachim Curtius, Norbert Maier, Theo Kurtén, Douglas R. Worsnop, Markku Kulmala, Matti Rissanen, Rainer Volkamer, Yee Jun Tham, Neil M. Donahue, and Mikko Sipilä
Atmos. Meas. Tech., 14, 4187–4202, https://doi.org/10.5194/amt-14-4187-2021, https://doi.org/10.5194/amt-14-4187-2021, 2021
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Atmospheric iodine species are often short-lived with low abundance and have thus been challenging to measure. We show that the bromide chemical ionization mass spectrometry, compatible with both the atmospheric pressure and reduced pressure interfaces, can simultaneously detect various gas-phase iodine species. Combining calibration experiments and quantum chemical calculations, we quantify detection sensitivities to HOI, HIO3, I2, and H2SO4, giving detection limits down to < 106 molec. cm-3.
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.
Clémence Rose, Matti P. Rissanen, Siddharth Iyer, Jonathan Duplissy, Chao Yan, John B. Nowak, Aurélie Colomb, Régis Dupuy, Xu-Cheng He, Janne Lampilahti, Yee Jun Tham, Daniela Wimmer, Jean-Marc Metzger, Pierre Tulet, Jérôme Brioude, Céline Planche, Markku Kulmala, and Karine Sellegri
Atmos. Chem. Phys., 21, 4541–4560, https://doi.org/10.5194/acp-21-4541-2021, https://doi.org/10.5194/acp-21-4541-2021, 2021
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Sulfuric acid (H2SO4) is commonly accepted as a key precursor for atmospheric new particle formation. However, direct measurements of [H2SO4] remain challenging, motivating the development of proxies. Using data collected in two different volcanic plumes, we show, under these specific conditions, the good performance of a proxy from the literature and also highlight the benefit of the newly developed proxies for the prediction of the highest [H2SO4] values.
Martin Heinritzi, Lubna Dada, Mario Simon, Dominik Stolzenburg, Andrea C. Wagner, Lukas Fischer, Lauri R. Ahonen, Stavros Amanatidis, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Bernhard Baumgartner, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, Antonio Dias, Josef Dommen, Jonathan Duplissy, Henning Finkenzeller, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Manuel Granzin, Imad El Haddad, Xucheng He, Johanna Helm, Victoria Hofbauer, Christopher R. Hoyle, Juha Kangasluoma, Timo Keber, Changhyuk Kim, Andreas Kürten, Houssni Lamkaddam, Tiia M. Laurila, Janne Lampilahti, Chuan Ping Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Vladimir Makhmutov, Hanna Elina Manninen, Ruby Marten, Serge Mathot, Roy Lee Mauldin, Bernhard Mentler, Ugo Molteni, Tatjana Müller, Wei Nie, Tuomo Nieminen, Antti Onnela, Eva Partoll, Monica Passananti, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti P. Rissanen, Clémence Rose, Siegfried Schobesberger, Wiebke Scholz, Kay Scholze, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, Miguel Vazquez-Pufleau, Annele Virtanen, Alexander L. Vogel, Rainer Volkamer, Robert Wagner, Mingyi Wang, Lena Weitz, Daniela Wimmer, Mao Xiao, Chao Yan, Penglin Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Urs Baltensperger, Armin Hansel, Markku Kulmala, António Tomé, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 11809–11821, https://doi.org/10.5194/acp-20-11809-2020, https://doi.org/10.5194/acp-20-11809-2020, 2020
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With experiments performed at CLOUD, we show how isoprene interferes in monoterpene oxidation via RO2 termination at atmospherically relevant concentrations. This interference shifts the distribution of highly oxygenated organic molecules (HOMs) away from C20 class dimers towards C15 class dimers, which subsequently reduces both biogenic nucleation and early growth rates. Our results may help to understand the absence of new-particle formation in isoprene-rich environments.
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.
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.
Dean Chen, Putian Zhou, Tuomo Nieminen, Pontus Roldin, Ximeng Qi, Petri Clusius, Carlton Xavier, Lukas Pichelstorfer, Markku Kulmala, Pekka Rantala, Juho Aalto, Nina Sarnela, Pasi Kolari, Petri Keronen, Matti P. Rissanen, Metin Baykara, and Michael Boy
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-128, https://doi.org/10.5194/acp-2020-128, 2020
Preprint withdrawn
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Atmospheric oxidants OH, O3 and NO3 dominate the atmospheric oxidation capacity, and sulfuric acid (H2SO4) is considered as a main driver for new particle formation events. We studied how the trends of these atmospheric oxidants and H2SO4 changed in southern Finland during the past 12 years and discussed how these trends related to decreasing emissions of air pollutants in Europe. Our results showed that OH increased by 1.56 % yr−1 at daytime and NO3 decreased by 3.92 % yr−1 at nighttime.
Olga Garmash, Matti P. Rissanen, Iida Pullinen, Sebastian Schmitt, Oskari Kausiala, Ralf Tillmann, Defeng Zhao, Carl Percival, Thomas J. Bannan, Michael Priestley, Åsa M. Hallquist, Einhard Kleist, Astrid Kiendler-Scharr, Mattias Hallquist, Torsten Berndt, Gordon McFiggans, Jürgen Wildt, Thomas F. Mentel, and Mikael Ehn
Atmos. Chem. Phys., 20, 515–537, https://doi.org/10.5194/acp-20-515-2020, https://doi.org/10.5194/acp-20-515-2020, 2020
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Highly oxygenated organic molecules (HOMs) facilitate aerosol formation in the atmosphere. Using NO3− chemical ionization mass spectrometry we investigated HOM composition and yield in oxidation of aromatic compounds at different reactant concentrations, in the presence of NOx and seed aerosol. Higher OH concentrations increased HOM yield, suggesting multiple oxidation steps, and affected HOM composition, potentially explaining in part discrepancies in published secondary organic aerosol yields.
Ximeng Qi, Aijun Ding, Pontus Roldin, Zhengning Xu, Putian Zhou, Nina Sarnela, Wei Nie, Xin Huang, Anton Rusanen, Mikael Ehn, Matti P. Rissanen, Tuukka Petäjä, Markku Kulmala, and Michael Boy
Atmos. Chem. Phys., 18, 11779–11791, https://doi.org/10.5194/acp-18-11779-2018, https://doi.org/10.5194/acp-18-11779-2018, 2018
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In this study we simulate the HOM concentrations and discuss their roles in NPF at a remote boreal forest site in Finland and a suburban site in eastern China. We found that sulfuric acid and HOM organonitrate concentrations in the gas phase are significantly higher but other HOM monomers and dimers from monoterpene oxidation are lower in eastern China. This study highlights the need for molecular-scale measurements in improving the understanding of NPF mechanisms in polluted areas.
Nina Sarnela, Tuija Jokinen, Jonathan Duplissy, Chao Yan, Tuomo Nieminen, Mikael Ehn, Siegfried Schobesberger, Martin Heinritzi, Sebastian Ehrhart, Katrianne Lehtipalo, Jasmin Tröstl, Mario Simon, Andreas Kürten, Markus Leiminger, Michael J. Lawler, Matti P. Rissanen, Federico Bianchi, Arnaud P. Praplan, Jani Hakala, Antonio Amorim, Marc Gonin, Armin Hansel, Jasper Kirkby, Josef Dommen, Joachim Curtius, James N. Smith, Tuukka Petäjä, Douglas R. Worsnop, Markku Kulmala, Neil M. Donahue, and Mikko Sipilä
Atmos. Chem. Phys., 18, 2363–2380, https://doi.org/10.5194/acp-18-2363-2018, https://doi.org/10.5194/acp-18-2363-2018, 2018
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Atmospheric trace gases can form small molecular clusters, which can grow to larger sizes through the condensation of vapours. This process is called new particle formation. In this paper we studied the formation of sulfuric acid and highly oxygenated molecules, the key compounds in atmospheric new particle formation, in chamber experiments and introduced a way to simulate these ozonolysis products of α-pinene in a simple manner.
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.
Xuemeng Chen, Lauriane L. J. Quéléver, Pak L. Fung, Jutta Kesti, Matti P. Rissanen, Jaana Bäck, Petri Keronen, Heikki Junninen, Tuukka Petäjä, Veli-Matti Kerminen, and Markku Kulmala
Atmos. Chem. Phys., 18, 49–63, https://doi.org/10.5194/acp-18-49-2018, https://doi.org/10.5194/acp-18-49-2018, 2018
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We analysed a 20-year-long dataset collected in a Finnish boreal forest at SMEAR II station to investigate the frequency and strength of ozone depletion events. We could identify a number of ozone depletion events that lasted for more than 3 h, mainly in the autumn and winter months. Their occurrence was likely related to the formation of a low mixing layer under the conditions of low temperatures, low wind speeds, high relative humidities and limited intensity of solar radiation.
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
Putian Zhou, Laurens Ganzeveld, Ditte Taipale, Üllar Rannik, Pekka Rantala, Matti Petteri Rissanen, Dean Chen, and Michael Boy
Atmos. Chem. Phys., 17, 14309–14332, https://doi.org/10.5194/acp-17-14309-2017, https://doi.org/10.5194/acp-17-14309-2017, 2017
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In boreal forest, there is a large number of gaseous organic compounds called biogenic volatile organic compounds (BVOCs). Within the canopy, they can be emitted from vegetation and soil, react with each other and other gases, be transported in the air, and be removed from vegetation and soil surfaces. We applied a numerical model to simulate these processes and found that these BVOCs can be divided into five categories according to the significance of their sources and sinks.
Federico Bianchi, Olga Garmash, Xucheng He, Chao Yan, Siddharth Iyer, Ida Rosendahl, Zhengning Xu, Matti P. Rissanen, Matthieu Riva, Risto Taipale, Nina Sarnela, Tuukka Petäjä, Douglas R. Worsnop, Markku Kulmala, Mikael Ehn, and Heikki Junninen
Atmos. Chem. Phys., 17, 13819–13831, https://doi.org/10.5194/acp-17-13819-2017, https://doi.org/10.5194/acp-17-13819-2017, 2017
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Naturally charged highly oxidised molecules (HOMs) were characterized using advanced mass spectrometers. Two different classes of compounds, clustered with the nitrate and bisulfate ions, were identified: HOMs containing only carbon, hydrogen and oxygen and nitrogen-containing HOMs or organonitrates (ONs). They exhibit strong diurnal variations where HOMs peak during night and ONs during day. Finally, large clusters containing up to 40 carbon atoms (four oxidized
α-pinene units) were observed.
Emilie Öström, Zhou Putian, Guy Schurgers, Mikhail Mishurov, Niku Kivekäs, Heikki Lihavainen, Mikael Ehn, Matti P. Rissanen, Theo Kurtén, Michael Boy, Erik Swietlicki, and Pontus Roldin
Atmos. Chem. Phys., 17, 8887–8901, https://doi.org/10.5194/acp-17-8887-2017, https://doi.org/10.5194/acp-17-8887-2017, 2017
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We used a model to study how biogenic volatile organic compounds (BVOCs) emitted from the boreal forest contribute to the formation and growth of particles in the atmosphere. Some of these particles are important climate forcers, acting as seeds for cloud droplet fomation. We implemented a new gas chemistry mechanism that describes how the BVOCs are oxidized and form low-volatility highly oxidized organic molecules. With the new mechanism we are able to accurately predict the particle growth.
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.
Chao Yan, Wei Nie, Mikko Äijälä, Matti P. Rissanen, Manjula R. Canagaratna, Paola Massoli, Heikki Junninen, Tuija Jokinen, Nina Sarnela, Silja A. K. Häme, Siegfried Schobesberger, Francesco Canonaco, Lei Yao, André S. H. Prévôt, Tuukka Petäjä, Markku Kulmala, Mikko Sipilä, Douglas R. Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 16, 12715–12731, https://doi.org/10.5194/acp-16-12715-2016, https://doi.org/10.5194/acp-16-12715-2016, 2016
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Highly oxidized multifunctional compounds (HOMs) are known to have a significant contribution to secondary aerosol formation, yet their dominating formation pathways remain unclear in the atmosphere. We apply positive matrix factorization (PMF) on HOM data, and successfully retrieve factors representing different formation pathways. The results improve our understanding of HOM formation, and provide new perspectives on using PMF to study the variation of short-lived specie.
Felipe D. Lopez-Hilfiker, Siddarth Iyer, Claudia Mohr, Ben H. Lee, Emma L. D'Ambro, Theo Kurtén, and Joel A. Thornton
Atmos. Meas. Tech., 9, 1505–1512, https://doi.org/10.5194/amt-9-1505-2016, https://doi.org/10.5194/amt-9-1505-2016, 2016
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We present the maximum sensitivity of a TOF-CIMS using the collision limit and iodide adducts. We also present an ion adduct declustering scanning procedure which determines the effective binding energies of the detected ion adducts and therefore their approximate sensitivity. The combination of declustering scanning and the collision limit provides an approximate calibration for many compounds in the mass spectrum which would otherwise be impossible to obtain by traditional methods.
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.
R. L. Mauldin III, M. P. Rissanen, T. Petäjä, and M. Kulmala
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2015-398, https://doi.org/10.5194/amt-2015-398, 2016
Revised manuscript not accepted
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The manuscript describes a novel instrument for the measurement of OH, HO2+RO2, and other atmospheric species. The instrument described combines the chemical ionization techniques of nitrate CIMS, OH conversion to H2SO4, HO2+RO2 conversion to H2SO4, and high resolution time of flight mass spectroscopy into one system. By using one instrument to obtain spectra it is possible to compare spectra from the different modes and gain further chemical information towards peak identification.
M. Sipilä, N. Sarnela, T. Jokinen, H. Junninen, J. Hakala, M. P. Rissanen, A. Praplan, M. Simon, A. Kürten, F. Bianchi, J. Dommen, J. Curtius, T. Petäjä, and D. R. Worsnop
Atmos. Meas. Tech., 8, 4001–4011, https://doi.org/10.5194/amt-8-4001-2015, https://doi.org/10.5194/amt-8-4001-2015, 2015
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Atmospheric concentrations of amines are poorly known mainly due to challenges related to their reliable high-sensitivity detection. We have created a method and instrument that is capable for detecting amines with lowest limit of detection of around 0.01 parts per trillion. Application of the instrument in the field study indicates that concentrations of dimethyl amine in a boreal forest site are below 0.03ppt, not enough to account for the observed new particle formation rates.
T. F. Mentel, M. Springer, M. Ehn, E. Kleist, I. Pullinen, T. Kurtén, M. Rissanen, A. Wahner, and J. Wildt
Atmos. Chem. Phys., 15, 6745–6765, https://doi.org/10.5194/acp-15-6745-2015, https://doi.org/10.5194/acp-15-6745-2015, 2015
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We studied a series of cycloalkenes and methyl-substituted alkenes in order to elucidate the structural pre-requisites and chemical pathways to the recently discovered class of highly oxidized molecules ELVOC (Ehn et al., Nature, 2014). ELVOC may totally change the view on (parts of) the mechanism of SOA formation. We present results which support recent observations of H shifts from C-H to peroxy radicals, highlighting the pivotal role of peroxyradicals in organic atmospheric chemistry.
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.
M. Sipilä, T. Jokinen, T. Berndt, S. Richters, R. Makkonen, N. M. Donahue, R. L. Mauldin III, T. Kurtén, P. Paasonen, N. Sarnela, M. Ehn, H. Junninen, M. P. Rissanen, J. Thornton, F. Stratmann, H. Herrmann, D. R. Worsnop, M. Kulmala, V.-M. Kerminen, and T. Petäjä
Atmos. Chem. Phys., 14, 12143–12153, https://doi.org/10.5194/acp-14-12143-2014, https://doi.org/10.5194/acp-14-12143-2014, 2014
J. Kangasluoma, C. Kuang, D. Wimmer, M. P. Rissanen, K. Lehtipalo, M. Ehn, D. R. Worsnop, J. Wang, M. Kulmala, and T. Petäjä
Atmos. Meas. Tech., 7, 689–700, https://doi.org/10.5194/amt-7-689-2014, https://doi.org/10.5194/amt-7-689-2014, 2014
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Observing low-altitude features in ozone concentrations in a shoreline environment via uncrewed aerial systems
An integrated uncrewed aerial vehicle platform with sensing and sampling systems for the measurement of air pollutant concentrations
Design and evaluation of a low-cost sensor node for near-background methane measurement
Development of a Multichannel Organics In situ enviRonmental Analyzer (MOIRA) for mobile measurements of volatile organic compounds
Evaluation of Aeris mid-infrared absorption (MIRA), Picarro CRDS (cavity ring-down spectroscopy) G2307, and dinitrophenylhydrazine (DNPH)-based sampling for long-term formaldehyde monitoring efforts
Multi-decadal atmospheric carbon dioxide measurements in Central Europe, Hungary
A New Technique for Airborne Measurements to Quantify Methane Emissions Over a Wide Range: Implementation and Validation
Performance characterization of a laminar gas inlet
Validation and field application of a low-cost device to measure CO2 and evapotranspiration (ET) fluxes
Identifying and correcting interferences to PTR-ToF-MS measurements of isoprene and other urban volatile organic compounds
Development of a continuous UAV-mounted air sampler and application to the quantification of CO2 and CH4 emissions from a major coking plant
Uptake behavior of polycyclic aromatic compounds during field calibrations of the XAD-based passive air sampler across seasons and locations
Drone CO2 Measurements During the Tajogaite Volcanic Eruption
New infrared spectroscopy instrument for reliable low humidity water vapour isotopic composition measurements
Using metal oxide gas sensors for the estimate of methane controlled releases: reconstruction of the methane mole fraction time-series and quantification of the release rates and locations
Effect of land–sea air mass transport on spatiotemporal distributions of atmospheric CO2 and CH4 mixing ratios over the southern Yellow Sea
HYPHOP: a tool for high-altitude, long-range monitoring of hydrogen peroxide and higher organic peroxides in the atmosphere
Portable, low-cost samplers for distributed sampling of atmospheric gases
SI-traceable validation of a laser spectrometer for balloon-borne measurements of water vapor in the upper atmosphere
Toward on-demand measurements of greenhouse gas emissions using an uncrewed aircraft Aircore system
Field evaluation of low-cost electrochemical air quality gas sensors under extreme temperature and relative humidity conditions
A novel, cost-effective analytical method for measuring high-resolution vertical profiles of stratospheric trace gases using a gas chromatograph coupled with an electron capture detector
Ethylene oxide monitor with part-per-trillion precision for in situ measurements
Development of an automated pump-efficiency measuring system for ozonesondes utilizing an airbag-type flowmeter
Short-term variability of atmospheric helium revealed through a cryo-enrichment method
Using tunable infrared laser direct absorption spectroscopy for ambient hydrogen chloride detection: HCl-TILDAS
New methods for the calibration of optical resonators: integrated calibration by means of optical modulation (ICOM) and narrow-band cavity ring-down (NB-CRD)
A modular field system for near-surface, vertical profiling of the atmospheric composition in harsh environments using cavity ring-down spectroscopy
Field comparison of two novel open-path instruments that measure dry deposition and emission of ammonia using flux-gradient and eddy covariance methods
Development of multi-channel whole-air sampling equipment onboard an unmanned aerial vehicle for investigating volatile organic compounds' vertical distribution in the planetary boundary layer
Electrochemical sensors on board a Zeppelin NT: in-flight evaluation of low-cost trace gas measurements
Evaluating the performance of a Picarro G2207-i analyser for high-precision atmospheric O2 measurements
Airborne flux measurements of ammonia over the southern Great Plains using chemical ionization mass spectrometry
Optical receiver characterizations and corrections for ground-based and airborne measurements of spectral actinic flux densities
Development and validation of a new in situ technique to measure total gaseous chlorine in air
True eddy accumulation – Part 1: Solutions to the problem of non-vanishing mean vertical wind velocity
True eddy accumulation – Part 2: Theory and experiment of the short-time eddy accumulation method
A simultaneous CH4 and CO2 flux quantification method for industrial site emissions from in-situ concentration measurements on-board an Unmanned Aircraft Vehicle
Chemical ionization mass spectrometry utilizing ammonium ions (NH4+ CIMS) for measurements of organic compounds in the atmosphere
Direct measurement of N2O5 heterogeneous uptake coefficients on ambient aerosols via an aerosol flow tube system: design, characterization and performance
Online measurements of cycloalkanes based on NO+ chemical ionization in proton transfer reaction time-of-flight mass spectrometry (PTR-ToF-MS)
Intercomparison of in situ measurements of ambient NH3: instrument performance and application under field conditions
A lightweight broadband cavity-enhanced spectrometer for NO2 measurement on uncrewed aerial vehicles
On the development of a new prototype PTR-ToF-MS instrument and its application to the detection of atmospheric amines
Low-complexity methods to mitigate the impact of environmental variables on low-cost UAS-based atmospheric carbon dioxide measurements
Comparison of airborne measurements of NO, NO2, HONO, NOy, and CO during FIREX-AQ
Development of a broadband cavity-enhanced absorption spectrometer for simultaneous measurements of ambient NO3, NO2, and H2O
Sebastian Diez, Stuart Lacy, Hugh Coe, Josefina Urquiza, Max Priestman, Michael Flynn, Nicholas Marsden, Nicholas A. Martin, Stefan Gillott, Thomas Bannan, and Pete M. Edwards
Atmos. Meas. Tech., 17, 3809–3827, https://doi.org/10.5194/amt-17-3809-2024, https://doi.org/10.5194/amt-17-3809-2024, 2024
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In this paper we present an overview of the QUANT project, which to our knowledge is one of the largest evaluations of commercial sensors to date. The objective was to evaluate the performance of a range of commercial products and also to nourish the different applications in which these technologies can offer relevant information.
Linda Ort, Lenard Lukas Röder, Uwe Parchatka, Rainer Königstedt, Daniel Crowley, Frank Kunz, Ralf Wittkowski, Jos Lelieveld, and Horst Fischer
Atmos. Meas. Tech., 17, 3553–3565, https://doi.org/10.5194/amt-17-3553-2024, https://doi.org/10.5194/amt-17-3553-2024, 2024
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Airborne in situ measurements are of great importance to collect valuable data to improve our knowledge of the atmosphere but also present challenges which demand specific designs. This study presents an IR spectrometer for airborne trace-gas measurements with high data efficiency and a simple, compact design. Its in-flight performance is characterized with the help of a test flight and a comparison with another spectrometer. Moreover, results from its first campaign highlight its benefits.
Roger Curcoll, Claudia Grossi, Stefan Röttger, and Arturo Vargas
Atmos. Meas. Tech., 17, 3047–3065, https://doi.org/10.5194/amt-17-3047-2024, https://doi.org/10.5194/amt-17-3047-2024, 2024
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This paper presents a new user-friendly version of the Atmospheric Radon MONitor (ARMON). The efficiency of the instrument is of 0.0057 s-1, obtained using different techniques at Spanish and German chambers. The total calculated uncertainty of the ARMON for hourly radon concentrations above 5 Bq m-3 is lower than 10 % (k = 1). Results confirm that the ARMON is suitable to measure low-level radon activity concentrations and to be used as a transfer standard to calibrate in situ radon monitors.
Josie K. Radtke, Benjamin N. Kies, Whitney A. Mottishaw, Sydney M. Zeuli, Aidan T. H. Voon, Kelly L. Koerber, Grant W. Petty, Michael P. Vermeuel, Timothy H. Bertram, Ankur R. Desai, Joseph P. Hupy, R. Bradley Pierce, Timothy J. Wagner, and Patricia A. Cleary
Atmos. Meas. Tech., 17, 2833–2847, https://doi.org/10.5194/amt-17-2833-2024, https://doi.org/10.5194/amt-17-2833-2024, 2024
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The use of uncrewed aircraft systems (UASs) to conduct a vertical profiling of ozone and meteorological variables was evaluated using comparisons between tower or ground observations and UAS-based measurements. Changes to the UAS profiler showed an improvement in performance. The profiler was used to see the impact of Chicago pollution plumes on a shoreline area near Lake Michigan.
Chen-Wei Liang and Chang-Hung Shen
Atmos. Meas. Tech., 17, 2671–2686, https://doi.org/10.5194/amt-17-2671-2024, https://doi.org/10.5194/amt-17-2671-2024, 2024
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In the present study, a UAV platform with sensing and sampling systems was developed for 3D air pollutant concentration measurements. The sensing system of this platform contains multiple microsensors and IoT technologies for obtaining the real-time 3D distributions of critical air pollutants. The sampling system contains gas sampling sets and a 1 L Tedlar bag instead of a canister for the 3D measurement of VOC concentrations in accordance with the TO-15 method of the US EPA.
Daniel Furuta, Bruce Wilson, Albert A. Presto, and Jiayu Li
Atmos. Meas. Tech., 17, 2103–2121, https://doi.org/10.5194/amt-17-2103-2024, https://doi.org/10.5194/amt-17-2103-2024, 2024
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Methane is an important driver of climate change and is challenging to inexpensively sense in low atmospheric concentrations. We developed a low-cost sensor to monitor methane and tested it in indoor and outdoor settings. Our device shows promise for monitoring low levels of methane. We characterize its limitations and suggest future research directions for further development.
Audrey J. Dang, Nathan M. Kreisberg, Tyler L. Cargill, Jhao-Hong Chen, Sydney Hornitschek, Remy Hutheesing, Jay R. Turner, and Brent J. Williams
Atmos. Meas. Tech., 17, 2067–2087, https://doi.org/10.5194/amt-17-2067-2024, https://doi.org/10.5194/amt-17-2067-2024, 2024
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The Multichannel Organics In situ enviRonmental Analyzer (MOIRA) is a new instrument for measuring speciated volatile organic compounds (VOCs) in the air and has been developed for mapping concentrations from a hybrid car. MOIRA is characterized in the lab and pilot field studies of indoor air in a single-family residence and outdoor air during a mobile deployment. Future applications include indoor, outdoor, and lab measurements to grasp the impact of VOCs on air quality, health, and climate.
Asher P. Mouat, Zelda A. Siegel, and Jennifer Kaiser
Atmos. Meas. Tech., 17, 1979–1994, https://doi.org/10.5194/amt-17-1979-2024, https://doi.org/10.5194/amt-17-1979-2024, 2024
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Three fast-measurement formaldehyde monitors were deployed at two field sites in Atlanta, GA, over 1 year. Four different zeroing methods were tested to develop an optimal field setup as well as procedures for instrument calibration. Observations agreed well after calibration but were much higher compared to the TO-11A monitoring method, which is the golden standard. Historical HCHO concentrations were compared with measurements in this work, showing a 22 % reduction in midday HCHO since 1999.
László Haszpra
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2024-29, https://doi.org/10.5194/amt-2024-29, 2024
Revised manuscript accepted for AMT
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The paper evaluates a 30-year-long atmospheric CO2 data series from a mid-continental Central European site, Hegyhátsál (HUN). It presents the site-specific features observed in the long-term evolution of the atmospheric CO2 concentration. Since the measurement data are widely used in atmospheric inverse models and budget calculations all around the world, the paper provides potentially valuable information for model tuning and interpretation of the model results.
Jonathan F. Dooley, Kenneth Minschwaner, Manvendra K. Dubey, Sahar H. El Abbadi, Evan D. Sherwin, Aaron G. Meyer, Emily Follansbee, and James E. Lee
EGUsphere, https://doi.org/10.5194/egusphere-2024-760, https://doi.org/10.5194/egusphere-2024-760, 2024
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Methane is a powerful greenhouse gas originating from both natural and human activities. We describe a new Unmanned Aerial System (UAS) designed to measure methane emission rates from over a wide range of scales. This system has been used for direct quantification of point sources and distributed emitters over scales of up to 1 km. The system uses simultaneous measurements of methane and ethane to distinguish between different kinds of natural and human-related emission sources.
Da Yang, Margarita Reza, Roy Mauldin, Rainer Volkamer, and Suresh Dhaniyala
Atmos. Meas. Tech., 17, 1463–1474, https://doi.org/10.5194/amt-17-1463-2024, https://doi.org/10.5194/amt-17-1463-2024, 2024
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This paper evaluates the performance of an aircraft gas inlet. Here, we use computational fluid dynamics (CFD) and experiments to demonstrate the role of turbulence in determining sampling performance of a gas inlet and identify ideal conditions for inlet operation to minimize gas loss. Experiments conducted in a high-speed wind tunnel under near-aircraft speeds validated numerical results. We believe that the results obtained from this work will greatly inform future gas inlet studies.
Reena Macagga, Michael Asante, Geoffroy Sossa, Danica Antonijević, Maren Dubbert, and Mathias Hoffmann
Atmos. Meas. Tech., 17, 1317–1332, https://doi.org/10.5194/amt-17-1317-2024, https://doi.org/10.5194/amt-17-1317-2024, 2024
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Using only low-cost microcontrollers and sensors, we constructed a measurement device to accurately and precisely obtain atmospheric carbon dioxide and water fluxes. The device was tested against known concentration increases and high-cost, commercial sensors during a laboratory and field experiment. We additionally tested the device over a longer period in a field study in Ghana during which the net ecosystem carbon balance and water use efficiency of maize cultivation were studied.
Matthew M. Coggon, Chelsea E. Stockwell, Megan S. Claflin, Eva Y. Pfannerstill, Lu Xu, Jessica B. Gilman, Julia Marcantonio, Cong Cao, Kelvin Bates, Georgios I. Gkatzelis, Aaron Lamplugh, Erin F. Katz, Caleb Arata, Eric C. Apel, Rebecca S. Hornbrook, Felix Piel, Francesca Majluf, Donald R. Blake, Armin Wisthaler, Manjula Canagaratna, Brian M. Lerner, Allen H. Goldstein, John E. Mak, and Carsten Warneke
Atmos. Meas. Tech., 17, 801–825, https://doi.org/10.5194/amt-17-801-2024, https://doi.org/10.5194/amt-17-801-2024, 2024
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Mass spectrometry is a tool commonly used to measure air pollutants. This study evaluates measurement artifacts produced in the proton-transfer-reaction mass spectrometer. We provide methods to correct these biases and better measure compounds that degrade air quality.
Tianran Han, Conghui Xie, Yayong Liu, Yanrong Yang, Yuheng Zhang, Yufei Huang, Xiangyu Gao, Xiaohua Zhang, Fangmin Bao, and Shao-Meng Li
Atmos. Meas. Tech., 17, 677–691, https://doi.org/10.5194/amt-17-677-2024, https://doi.org/10.5194/amt-17-677-2024, 2024
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This study reported an integrated UAV measurement platform for GHG monitoring and its application for emission quantification from a coking plant. The key element of this system is a newly designed air sampler, consisting of a 150 m long tube with remote-controlled time stamping. When comparing the top-down results to those derived from the bottom-up inventory method, the present findings indicate that the use of IPCC emission factors for emission calculations can lead to overestimation.
Yuening Li, Faqiang Zhan, Yushan Su, Ying Duan Lei, Chubashini Shunthirasingham, Zilin Zhou, Jonathan P. D. Abbatt, Hayley Hung, and Frank Wania
Atmos. Meas. Tech., 17, 715–729, https://doi.org/10.5194/amt-17-715-2024, https://doi.org/10.5194/amt-17-715-2024, 2024
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A simple device for sampling gases from the atmosphere without the help of pumps was calibrated for an important group of hazardous air pollutants called polycyclic aromatic compounds (PACs). While the sampler appeared to perform well when used for relatively short periods of up to several months, some PACs were lost from the sampler during longer deployments. Sampling rates that can be used to quantitatively interpret the quantities of PACs taken up in the device have been derived.
John Ericksen, Tobias Fischer, G. Matthew Fricke, Scott Nowicki, Nemesio Pérez, Pedro Hernández Pérez, Eleazar Padrón González, and Melanie Moses
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2023-229, https://doi.org/10.5194/amt-2023-229, 2024
Revised manuscript accepted for AMT
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Volcanic eruptions emit significant quantities of carbon dioxide (CO2) to the atmosphere. We present a new method for directly determining the CO2 emission from a volcanic eruption using om La Palma Island, Spain using an unpiloted areal vehicle (UAV). We also collected samples of the emitted CO2 and analyzed their isotopic composition. Together with the emission rate the isotopic data provide valuable information on the state of volcanic activity and the potential evolution the eruption.
Mathieu Casado, Amaelle Landais, Tim Stoltmann, Justin Chaillot, Mathieu Daëron, Frédéric Prié, Baptiste Bordet, and Samir Kassi
EGUsphere, https://doi.org/10.5194/egusphere-2023-2457, https://doi.org/10.5194/egusphere-2023-2457, 2023
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Measuring water isotopic composition in Antarctica is difficult because of the extremely cold temperature in winter. Here, we designed a new infrared spectrometer able to measure the vapour isotopic composition more than 95 % of the year in the coldest locations of Antarctica, while current commercial instruments are only able to measure during the warm summer months in the interior.
Rodrigo Andres Rivera Martinez, Pramod Kumar, Olivier Laurent, Grégoire Broquet, Christopher Caldow, Ford Cropley, Diego Santaren, Adil Shah, Cécile Mallet, Michel Ramonet, Leonard Rivier, Catherine Juery, Olivier Duclaux, Caroline Bouchet, Elisa Allegrini, Hervé Utard, and Philippe Ciais
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2023-52, https://doi.org/10.5194/amt-2023-52, 2023
Revised manuscript accepted for AMT
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This study explores the use of Metal Oxide Sensors (MOS) as a low-cost alternative for detecting and measuring CH4 emissions from industrial facilities. MOS were exposed to several controlled releases to test their accuracy in detecting and quantifying emissions. Two reconstruction models were compared, and emission estimates were computed using a Gaussian dispersion model. Findings show that MOS can provide accurate emission estimates with a 25 % emission rate error and a 9.5 m location error.
Jiaxin Li, Kunpeng Zang, Yi Lin, Yuanyuan Chen, Shuo Liu, Shanshan Qiu, Kai Jiang, Xuemei Qing, Haoyu Xiong, Haixiang Hong, Shuangxi Fang, Honghui Xu, and Yujun Jiang
Atmos. Meas. Tech., 16, 4757–4768, https://doi.org/10.5194/amt-16-4757-2023, https://doi.org/10.5194/amt-16-4757-2023, 2023
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Based on observed data of CO2 and CH4 and meteorological parameters over the Yellow Sea in November 2012 and June 2013, a data process and quality control method was optimized and established to filter the data influenced by multiple factors. Spatial and seasonal variations in CO2 and CH4 mixing ratios were mainly controlled by the East Asian Monsoon, while the influence of air–sea exchange was slight.
Zaneta Hamryszczak, Antonia Hartmann, Dirk Dienhart, Sascha Hafermann, Bettina Brendel, Rainer Königstedt, Uwe Parchatka, Jos Lelieveld, and Horst Fischer
Atmos. Meas. Tech., 16, 4741–4756, https://doi.org/10.5194/amt-16-4741-2023, https://doi.org/10.5194/amt-16-4741-2023, 2023
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Hydroperoxide measurements improve the understanding of atmospheric oxidation processes. We introduce an instrumental setup for airborne measurements. The aim of the work is the characterization of the measurement method with emphasis on interferences impacting instrumental uncertainty. Technical and physical challenges do not critically impact the instrumental performance. The instrument resolves dynamic processes, such as convective transport, as shown based on the CAFE-Brazil campaign.
James F. Hurley, Alejandra Caceres, Deborah F. McGlynn, Mary E. Tovillo, Suzanne Pinar, Roger Schürch, Ksenia Onufrieva, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 16, 4681–4692, https://doi.org/10.5194/amt-16-4681-2023, https://doi.org/10.5194/amt-16-4681-2023, 2023
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Volatile organic compounds (VOCs) have a wide range of sources and impacts on environments and human health that make them spatially, temporally, and chemically varied. Current methods lack the ability to collect samples in ways that provide spatial and chemical resolution without complex, costly instrumentation. We describe and validate a low-cost, portable VOC sampler and demonstrate its utility in collecting distributed coordinated samples.
Simone Brunamonti, Manuel Graf, Tobias Bühlmann, Céline Pascale, Ivan Ilak, Lukas Emmenegger, and Béla Tuzson
Atmos. Meas. Tech., 16, 4391–4407, https://doi.org/10.5194/amt-16-4391-2023, https://doi.org/10.5194/amt-16-4391-2023, 2023
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The abundance of water vapor (H2O) in the upper atmosphere has a significant impact on the rate of global warming. We developed a new lightweight spectrometer (ALBATROSS) for H2O measurements aboard meteorological balloons. Here, we assess the accuracy and precision of ALBATROSS using metrology-grade reference gases. The results demonstrate the exceptional potential of mid-infrared laser absorption spectroscopy as a new reference method for in situ measurements of H2O in the upper atmosphere.
Zihan Zhu, Javier Gonzalez-Rocha, Yifan Ding, Isis Frausto-Vicencio, Sajjan Heerah, Akula Venkatram, Manvendra Dubey, Don Collins, and Francesca Hopkins
EGUsphere, https://doi.org/10.5194/egusphere-2023-1527, https://doi.org/10.5194/egusphere-2023-1527, 2023
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Increases in agriculture, oil and gas, and waste management activities have contributed to the growth of atmospheric methane levels and climate warming. In this manuscript, we explore the use of small uncrewed aircraft systems (sUAS) and Aircore technology to detect and quantify methane emissions. Results from field experiments demonstrate that sUAS and Aircore technology can be effective for detecting and quantifying methane emissions in near real-time.
Roubina Papaconstantinou, Marios Demosthenous, Spyros Bezantakos, Neoclis Hadjigeorgiou, Marinos Costi, Melina Stylianou, Elli Symeou, Chrysanthos Savvides, and George Biskos
Atmos. Meas. Tech., 16, 3313–3329, https://doi.org/10.5194/amt-16-3313-2023, https://doi.org/10.5194/amt-16-3313-2023, 2023
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In this paper, we investigate the performance of low-cost electrochemical gas sensors. We carried out yearlong measurements at a traffic air quality monitoring station, where the low-cost sensors were collocated with reference instruments and exposed to highly variable environmental conditions with extremely high temperatures and low relative humidity (RH). Sensors provide measurements that exhibit increasing errors and decreasing correlations as temperature increases and RH decreases.
Jianghanyang Li, Bianca C. Baier, Fred Moore, Tim Newberger, Sonja Wolter, Jack Higgs, Geoff Dutton, Eric Hintsa, Bradley Hall, and Colm Sweeney
Atmos. Meas. Tech., 16, 2851–2863, https://doi.org/10.5194/amt-16-2851-2023, https://doi.org/10.5194/amt-16-2851-2023, 2023
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Monitoring a suite of trace gases in the stratosphere will help us better understand the stratospheric circulation and its impact on the earth's radiation balance. However, such measurements are rare and usually expensive. We developed an instrument that can measure stratospheric trace gases using a low-cost sampling platform (AirCore). The results showed expected agreement with aircraft measurements, demonstrating this technique provides a low-cost and robust way to observe the stratosphere.
Tara I. Yacovitch, Christoph Dyroff, Joseph R. Roscioli, Conner Daube, J. Barry McManus, and Scott C. Herndon
Atmos. Meas. Tech., 16, 1915–1921, https://doi.org/10.5194/amt-16-1915-2023, https://doi.org/10.5194/amt-16-1915-2023, 2023
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Ethylene oxide is a toxic, carcinogenic compound used in the medical and bulk sterilization industry. Here we describe a precise and fast laser-based ethylene oxide monitor. We report months-long concentrations at a Massachusetts site, and we show how they suggest a potential emission source 35 km away. This source, and another, is confirmed by driving the instrument downwind of the sites, where concentrations were tens to tens of thousands of times greater than background levels.
Tatsumi Nakano and Takashi Morofuji
Atmos. Meas. Tech., 16, 1583–1595, https://doi.org/10.5194/amt-16-1583-2023, https://doi.org/10.5194/amt-16-1583-2023, 2023
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We have developed a system that can automatically measure the pump efficiency of the ECC-type ozonesonde. Operational measurement for 13 years by this system revealed that the efficiency fluctuates in each and slightly increases over time. Those can affect the estimation of total ozone amount by up to 4 %. This result indicates that it is necessary to understand the tendency of the pump correction factor of each ozonesonde in order to detect the actual atmospheric change with high accuracy.
Benjamin Birner, Eric Morgan, and Ralph F. Keeling
Atmos. Meas. Tech., 16, 1551–1561, https://doi.org/10.5194/amt-16-1551-2023, https://doi.org/10.5194/amt-16-1551-2023, 2023
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Atmospheric variations of helium (He) and CO2 are strongly linked due to the co-release of both gases from natural-gas burning. This implies that atmospheric He measurements may be a potentially powerful tool for verifying reported anthropogenic natural-gas usage. Here, we present the development and initial results of a novel measurement system of atmospheric He that paves the way for establishing a global monitoring network in the future.
John W. Halfacre, Jordan Stewart, Scott C. Herndon, Joseph R. Roscioli, Christoph Dyroff, Tara I. Yacovitch, Michael Flynn, Stephen J. Andrews, Steven S. Brown, Patrick R. Veres, and Pete M. Edwards
Atmos. Meas. Tech., 16, 1407–1429, https://doi.org/10.5194/amt-16-1407-2023, https://doi.org/10.5194/amt-16-1407-2023, 2023
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This study details a new sampling method for the optical detection of hydrogen chloride (HCl). HCl is an important atmospheric reservoir for chlorine atoms, which can affect nitrogen oxide cycling and the lifetimes of volatile organic compounds and ozone. However, HCl has a high affinity for interacting with surfaces, thereby preventing fast, quantitative measurements. The sampling technique in this study minimizes these surface interactions and provides a high-quality measurement of HCl.
Henning Finkenzeller, Denis Pöhler, Martin Horbanski, Johannes Lampel, and Ulrich Platt
Atmos. Meas. Tech., 16, 1343–1356, https://doi.org/10.5194/amt-16-1343-2023, https://doi.org/10.5194/amt-16-1343-2023, 2023
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Optical resonators enhance the light path in compact instruments, thereby improving their sensitivity. Determining the established path length in the instrument is a prerequisite for the accurate determination of trace gas concentrations but can be a significant complication in the use of such resonators. Here we show two calibration techniques which are relatively simple and free of consumables but still provide accurate calibrations. This facilitates the use of optical resonators.
Andrew W. Seidl, Harald Sodemann, and Hans Christian Steen-Larsen
Atmos. Meas. Tech., 16, 769–790, https://doi.org/10.5194/amt-16-769-2023, https://doi.org/10.5194/amt-16-769-2023, 2023
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It is challenging to make field measurements of stable water isotopes in the Arctic. To this end, we present a modular stable-water-isotope analyzer profiling system. The system operated for a 2-week field campaign on Svalbard during the Arctic winter. We evaluate the system’s performance and analyze any potential impact that the field conditions might have had on the isotopic measurements and the system's ability to resolve isotope gradients in the lowermost layer of the atmosphere.
Daan Swart, Jun Zhang, Shelley van der Graaf, Susanna Rutledge-Jonker, Arjan Hensen, Stijn Berkhout, Pascal Wintjen, René van der Hoff, Marty Haaima, Arnoud Frumau, Pim van den Bulk, Ruben Schulte, Margreet van Zanten, and Thomas van Goethem
Atmos. Meas. Tech., 16, 529–546, https://doi.org/10.5194/amt-16-529-2023, https://doi.org/10.5194/amt-16-529-2023, 2023
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During a 5-week comparison campaign, we tested two set-ups to measure half hourly ammonia fluxes. The eddy covariance and flux gradient systems showed very similar results when the upwind terrain was both homogeneous and free of obstacles. We discuss the technical performance and practical limitations of both systems. Measurements from these instruments can facilitate the study of processes behind ammonia deposition, an important contributor to eutrophication and acidificationin natural areas.
Suding Yang, Xin Li, Limin Zeng, Xuena Yu, Ying Liu, Sihua Lu, Xiaofeng Huang, Dongmei Zhang, Haibin Xu, Shuchen Lin, Hefan Liu, Miao Feng, Danlin Song, Qinwen Tan, Jinhui Cui, Lifan Wang, Ying Chen, Wenjie Wang, Haijiong Sun, Mengdi Song, Liuwei Kong, Yi Liu, Linhui Wei, Xianwu Zhu, and Yuanhang Zhang
Atmos. Meas. Tech., 16, 501–512, https://doi.org/10.5194/amt-16-501-2023, https://doi.org/10.5194/amt-16-501-2023, 2023
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Vertical observation of volatile organic compounds (VOCs) is essential to study the spatial distribution and evolution patterns of VOCs in the planetary boundary layer (PBL). This paper describes multi-channel whole-air sampling equipment onboard an unmanned aerial vehicle (UAV) for near-continuous VOC vertical observation. Vertical profiles of VOCs and trace gases during the evolution of the PBL in south-western China have been successfully obtained by deploying the newly developed UAV system.
Tobias Schuldt, Georgios I. Gkatzelis, Christian Wesolek, Franz Rohrer, Benjamin Winter, Thomas A. J. Kuhlbusch, Astrid Kiendler-Scharr, and Ralf Tillmann
Atmos. Meas. Tech., 16, 373–386, https://doi.org/10.5194/amt-16-373-2023, https://doi.org/10.5194/amt-16-373-2023, 2023
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We report in situ measurements of air pollutant concentrations within the planetary boundary layer on board a Zeppelin NT in Germany. We highlight the in-flight evaluation of electrochemical sensors that were installed inside a hatch box located on the bottom of the Zeppelin. Results from this work emphasize the potential of these sensors for other in situ airborne applications, e.g., on board unmanned aerial vehicles (UAVs).
Leigh S. Fleming, Andrew C. Manning, Penelope A. Pickers, Grant L. Forster, and Alex J. Etchells
Atmos. Meas. Tech., 16, 387–401, https://doi.org/10.5194/amt-16-387-2023, https://doi.org/10.5194/amt-16-387-2023, 2023
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Measurements of atmospheric O2 can help constrain the carbon cycle processes and quantify fossil fuel CO2 emissions; however, measurement of atmospheric O2 is very challenging, and existing analysers are complex systems to build and maintain. We have tested a new O2 analyser (Picarro Inc. G2207-i) in the laboratory and at Weybourne Atmospheric Observatory. We have found that the G2207-i does not perform as well as an existing O2 analyser from Sable Systems Inc.
Siegfried Schobesberger, Emma L. D'Ambro, Lejish Vettikkat, Ben H. Lee, Qiaoyun Peng, David M. Bell, John E. Shilling, Manish Shrivastava, Mikhail Pekour, Jerome Fast, and Joel A. Thornton
Atmos. Meas. Tech., 16, 247–271, https://doi.org/10.5194/amt-16-247-2023, https://doi.org/10.5194/amt-16-247-2023, 2023
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We present a new, highly sensitive technique for measuring atmospheric ammonia, an important trace gas that is emitted mainly by agriculture. We deployed the instrument on an aircraft during research flights over rural Oklahoma. Due to its fast response, we could analyze correlations with turbulent winds and calculate ammonia emissions from nearby areas at 1 to 2 km resolution. We observed high spatial variability and point sources that are not resolved in the US National Emissions Inventory.
Birger Bohn and Insa Lohse
Atmos. Meas. Tech., 16, 209–233, https://doi.org/10.5194/amt-16-209-2023, https://doi.org/10.5194/amt-16-209-2023, 2023
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Optical receivers for solar spectral actinic radiation are designed for angle-independent sensitivities within a hemisphere. Remaining imperfections can be compensated for by receiver-specific corrections based on laboratory characterizations and radiative transfer calculations of spectral radiance distributions. The corrections cover a wide range of realistic atmospheric conditions and were applied to ground-based and airborne measurements in a wavelength range 280–660 nm.
Teles C. Furlani, RenXi Ye, Jordan Stewart, Leigh R. Crilley, Peter M. Edwards, Tara F. Kahan, and Cora J. Young
Atmos. Meas. Tech., 16, 181–193, https://doi.org/10.5194/amt-16-181-2023, https://doi.org/10.5194/amt-16-181-2023, 2023
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This study describes a new technique to measure total gaseous chlorine, which is the sum of gas-phase chlorine-containing chemicals. The method converts any chlorine-containing molecule to hydrogen chloride that can be detected in real time using a cavity ring-down spectrometer. The new method was validated through laboratory experiments, as well as by making measurements of ambient outdoor air and indoor air during cleaning with a chlorine-based cleaner.
Anas Emad and Lukas Siebicke
Atmos. Meas. Tech., 16, 29–40, https://doi.org/10.5194/amt-16-29-2023, https://doi.org/10.5194/amt-16-29-2023, 2023
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The true eddy accumulation (TEA) method enables measuring atmospheric exchange with slow-response gas analyzers. TEA is formulated assuming ideal conditions with a zero mean vertical wind velocity during the averaging interval. This core assumption is rarely valid under field conditions. Here, we extend the TEA equation to accommodate nonideal conditions. The new equation allows constraining the systematic error term in the measured fluxes and the possibility to minimize or remove it.
Anas Emad and Lukas Siebicke
Atmos. Meas. Tech., 16, 41–55, https://doi.org/10.5194/amt-16-41-2023, https://doi.org/10.5194/amt-16-41-2023, 2023
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A new micrometeorological method to measure atmospheric exchange is proposed, and a prototype sampler is evaluated. The new method, called short-time eddy accumulation, is a variant of the eddy accumulation method, which is suited for use with slow gas analyzers. The new method enables adaptive time-varying accumulation intervals, which brings many advantages to flux measurements such as an improved dynamic range and the ability to run eddy accumulation in a continuous flow-through mode.
Jean-Louis Bonne, Ludovic Donnat, Grégory Albora, Jérémie Burgalat, Nicolas Chauvin, Delphine Combaz, Julien Cousin, Thomas Decarpenterie, Olivier Duclaux, Nicolas Dumelié, Nicolas Galas, Catherine Juery, Florian Parent, Florent Pineau, Abel Maunoury, Olivier Ventre, Marie-France Bénassy, and Lilian Joly
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2022-334, https://doi.org/10.5194/amt-2022-334, 2023
Revised manuscript accepted for AMT
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We present a top-down approach to quantify CO2 and CH4 emissions at the scale of an industrial site, based on a mass balance model relying on atmospheric concentrations measurements from a new sensor embarked on-board Unmanned Aircraft Vehicles (UAVs). We present a laboratory characterization of our sensor and a field validation of our quantification method, together with field application to the monitoring of two real-world offshore oil and gas platforms.
Lu Xu, Matthew M. Coggon, Chelsea E. Stockwell, Jessica B. Gilman, Michael A. Robinson, Martin Breitenlechner, Aaron Lamplugh, John D. Crounse, Paul O. Wennberg, J. Andrew Neuman, Gordon A. Novak, Patrick R. Veres, Steven S. Brown, and Carsten Warneke
Atmos. Meas. Tech., 15, 7353–7373, https://doi.org/10.5194/amt-15-7353-2022, https://doi.org/10.5194/amt-15-7353-2022, 2022
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We describe the development and operation of a chemical ionization mass spectrometer using an ammonium–water cluster (NH4+·H2O) as a reagent ion. NH4+·H2O is a highly versatile reagent ion for measurements of a wide range of oxygenated organic compounds. The major product ion is the cluster with NH4+ produced via ligand-switching reactions. The instrumental sensitivities of analytes depend on the binding energy of the analyte–NH4+ cluster; sensitivities can be estimated using voltage scanning.
Xiaorui Chen, Haichao Wang, Tianyu Zhai, Chunmeng Li, and Keding Lu
Atmos. Meas. Tech., 15, 7019–7037, https://doi.org/10.5194/amt-15-7019-2022, https://doi.org/10.5194/amt-15-7019-2022, 2022
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N2O5 is an important reservoir of atmospheric nitrogen, on whose interface reaction ambient particles can largely influence the fate of nitrogen oxides and air quality. In this study, we develop an approach to enable the reactions of N2O5 on ambient particles directly in a tube reactor, deriving the reaction rates with high accuracy by means of a chemistry model. Its successful application helps complement the data scarcity and to fill the knowledge gap between laboratory and field results.
Yubin Chen, Bin Yuan, Chaomin Wang, Sihang Wang, Xianjun He, Caihong Wu, Xin Song, Yibo Huangfu, Xiao-Bing Li, Yijia Liao, and Min Shao
Atmos. Meas. Tech., 15, 6935–6947, https://doi.org/10.5194/amt-15-6935-2022, https://doi.org/10.5194/amt-15-6935-2022, 2022
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In this study, we demonstrate that selective online measurements of cycloalkanes can be achieved using proton transfer reaction time-of-flight mass spectrometry with NO+ chemical ionization (NO+ PTR-ToF-MS), with fast response and low detection limits. Applications of this method in both urban air and emission sources will be shown.
Marsailidh M. Twigg, Augustinus J. C. Berkhout, Nicholas Cowan, Sabine Crunaire, Enrico Dammers, Volker Ebert, Vincent Gaudion, Marty Haaima, Christoph Häni, Lewis John, Matthew R. Jones, Bjorn Kamps, John Kentisbeer, Thomas Kupper, Sarah R. Leeson, Daiana Leuenberger, Nils O. B. Lüttschwager, Ulla Makkonen, Nicholas A. Martin, David Missler, Duncan Mounsor, Albrecht Neftel, Chad Nelson, Eiko Nemitz, Rutger Oudwater, Celine Pascale, Jean-Eudes Petit, Andrea Pogany, Nathalie Redon, Jörg Sintermann, Amy Stephens, Mark A. Sutton, Yuk S. Tang, Rens Zijlmans, Christine F. Braban, and Bernhard Niederhauser
Atmos. Meas. Tech., 15, 6755–6787, https://doi.org/10.5194/amt-15-6755-2022, https://doi.org/10.5194/amt-15-6755-2022, 2022
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Ammonia (NH3) gas in the atmosphere impacts the environment, human health, and, indirectly, climate. Historic NH3 monitoring was labour intensive, and the instruments were complicated. Over the last decade, there has been a rapid technology development, including “plug-and-play” instruments. This study is an extensive field comparison of the currently available technologies and provides evidence that for routine monitoring, standard operating protocols are required for datasets to be comparable.
Caroline C. Womack, Steven S. Brown, Steven J. Ciciora, Ru-Shan Gao, Richard J. McLaughlin, Michael A. Robinson, Yinon Rudich, and Rebecca A. Washenfelder
Atmos. Meas. Tech., 15, 6643–6652, https://doi.org/10.5194/amt-15-6643-2022, https://doi.org/10.5194/amt-15-6643-2022, 2022
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We present a new miniature instrument to measure nitrogen dioxide (NO2) using cavity-enhanced spectroscopy. NO2 contributes to the formation of pollutants such as ozone and particulate matter, and its concentration can vary widely near sources. We developed this lightweight (3.05 kg) low-power (<35 W) instrument to measure NO2 on uncrewed aircraft vehicles (UAVs) and demonstrate that it has the accuracy and precision needed for atmospheric field measurements.
Alexander Håland, Tomáš Mikoviny, Elisabeth Emilie Syse, and Armin Wisthaler
Atmos. Meas. Tech., 15, 6297–6307, https://doi.org/10.5194/amt-15-6297-2022, https://doi.org/10.5194/amt-15-6297-2022, 2022
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PTR-MS is widely used in atmospheric sciences for the detection of non-methane organic trace gases. The two most widely used types of PTR-MS instruments differ in their ion source and drift tube design. We herein present a new prototype PTR-MS instrument that hybridizes these designs and combines a conventional hollow cathode glow discharge ion source with a focusing ion–molecule reactor. We also show how this new instrument performs in detecting atmospheric amines.
Gustavo Britto Hupsel de Azevedo, Bill Doyle, Christopher A. Fiebrich, and David Schvartzman
Atmos. Meas. Tech., 15, 5599–5618, https://doi.org/10.5194/amt-15-5599-2022, https://doi.org/10.5194/amt-15-5599-2022, 2022
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Strong changes in pressure, temperature, and humidity occur when small scientific aircraft ascend through the atmosphere to measure carbon dioxide. These strong changes can produce errors in the carbon dioxide measurements. To avoid these errors, we present a low-cost and simple correction method. This low-complexity method allows more researchers to study atmospheric carbon dioxide, reducing entry barriers in this field.
Ilann Bourgeois, Jeff Peischl, J. Andrew Neuman, Steven S. Brown, Hannah M. Allen, Pedro Campuzano-Jost, Matthew M. Coggon, Joshua P. DiGangi, Glenn S. Diskin, Jessica B. Gilman, Georgios I. Gkatzelis, Hongyu Guo, Hannah A. Halliday, Thomas F. Hanisco, Christopher D. Holmes, L. Gregory Huey, Jose L. Jimenez, Aaron D. Lamplugh, Young Ro Lee, Jakob Lindaas, Richard H. Moore, Benjamin A. Nault, John B. Nowak, Demetrios Pagonis, Pamela S. Rickly, Michael A. Robinson, Andrew W. Rollins, Vanessa Selimovic, Jason M. St. Clair, David Tanner, Krystal T. Vasquez, Patrick R. Veres, Carsten Warneke, Paul O. Wennberg, Rebecca A. Washenfelder, Elizabeth B. Wiggins, Caroline C. Womack, Lu Xu, Kyle J. Zarzana, and Thomas B. Ryerson
Atmos. Meas. Tech., 15, 4901–4930, https://doi.org/10.5194/amt-15-4901-2022, https://doi.org/10.5194/amt-15-4901-2022, 2022
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Understanding fire emission impacts on the atmosphere is key to effective air quality management and requires accurate measurements. We present a comparison of airborne measurements of key atmospheric species in ambient air and in fire smoke. We show that most instruments performed within instrument uncertainties. In some cases, further work is needed to fully characterize instrument performance. Comparing independent measurements using different techniques is important to assess their accuracy.
Woohui Nam, Changmin Cho, Begie Perdigones, Tae Siek Rhee, and Kyung-Eun Min
Atmos. Meas. Tech., 15, 4473–4487, https://doi.org/10.5194/amt-15-4473-2022, https://doi.org/10.5194/amt-15-4473-2022, 2022
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We describe our vibration-resistant instrument for measuring ambient NO3, NO2, and H2O based on cavity-enhanced absorption spectroscopy. By simultaneous retrieval of H2O with the other species using a measured H2O absorption spectrum, direct quantifications among all species are possible without any pre-treatment for H2O. Our instrument achieves the effective light path to ~101.5 km, which allows the sensitive measurements of NO3 and NO2 as 1.41 pptv and 6.92 ppbv (1σ) in 1 s.
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Short summary
A novel chemical ionization methodology for rapid gas–phase environmental monitoring is presented. The usefulness of the new inlet design is demonstrated by measuring various aerosol precursor compounds that are present at very low concentrations by using two consecutive ionization schemes. This new inlet enables the detection of a wide range of compounds of interest with a minimum of effort and at a fast repetition rate.
A novel chemical ionization methodology for rapid gas–phase environmental monitoring is...
