Articles | Volume 22, issue 8
https://doi.org/10.5194/acp-22-5619-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-22-5619-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
27 Apr 2022
Research article |
| 27 Apr 2022
| 27 Apr 2022
Oxidation product characterization from ozonolysis of the diterpene ent-kaurene
Institute for Atmospheric and Earth System Research/Physics, Faculty
of Science, University of Helsinki, Helsinki, 00014, Finland
Olga Garmash
Institute for Atmospheric and Earth System Research/Physics, Faculty
of Science, University of Helsinki, Helsinki, 00014, Finland
Aerosol Physics Laboratory, Physics Unit, Tampere University, Tampere,
33014, Finland
Haiyan Li
Institute for Atmospheric and Earth System Research/Physics, Faculty
of Science, University of Helsinki, Helsinki, 00014, Finland
School of Civil and Environmental Engineering, Harbin Institute of
Technology, Shenzhen, 518055, China
Frans Graeffe
Institute for Atmospheric and Earth System Research/Physics, Faculty
of Science, University of Helsinki, Helsinki, 00014, Finland
Arnaud P. Praplan
Atmospheric Composition Research, Finnish Meteorological Institute,
Helsinki, 00101, Finland
Anssi Liikanen
Atmospheric Composition Research, Finnish Meteorological Institute,
Helsinki, 00101, Finland
Yanjun Zhang
Institute for Atmospheric and Earth System Research/Physics, Faculty
of Science, University of Helsinki, Helsinki, 00014, Finland
Université Claude Bernard Lyon 1, CNRS, IRCELYON,
Villeurbanne, 69626, France
Melissa Meder
Institute for Atmospheric and Earth System Research/Physics, Faculty
of Science, University of Helsinki, Helsinki, 00014, Finland
Otso Peräkylä
Institute for Atmospheric and Earth System Research/Physics, Faculty
of Science, University of Helsinki, Helsinki, 00014, Finland
Josep Peñuelas
Centre for Research on Ecology and Forestry Applications (CREAF), Bellaterra (Cerdanyola del Vallès), Catalonia, 08193, Spain
Consejo Superior de Investigaciones Científicas (CSIC), Global Ecology Unit, CREAF-CSIC-UAB, Bellaterra (Cerdanyola del
Vallès), Catalonia, 08193, Spain
Ana María Yáñez-Serrano
Centre for Research on Ecology and Forestry Applications (CREAF), Bellaterra (Cerdanyola del Vallès), Catalonia, 08193, Spain
Consejo Superior de Investigaciones Científicas (CSIC), Global Ecology Unit, CREAF-CSIC-UAB, Bellaterra (Cerdanyola del
Vallès), Catalonia, 08193, Spain
Institute of Environmental Assessment and Water Research (IDAEA)-CSIC, Barcelona, 08034, Spain
Institute for Atmospheric and Earth System Research/Physics, Faculty
of Science, University of Helsinki, Helsinki, 00014, Finland
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N-containing oxygenated organic molecules have been identified as important precursors of aerosol particles. We used an ultra-high-resolution mass spectrometer coupled with an online sample inlet to accurately measure their molecular composition, concentration level and variation patterns. We show their formation process and influencing factors in a Chinese megacity involving various volatile organic compound precursors and atmospheric oxidants, and we highlight the influence of PM2.5 episodes.
Sanna Saarikoski, Heidi Hellén, Arnaud P. Praplan, Simon Schallhart, Petri Clusius, Jarkko V. Niemi, Anu Kousa, Toni Tykkä, Rostislav Kouznetsov, Minna Aurela, Laura Salo, Topi Rönkkö, Luis M. F. Barreira, Liisa Pirjola, and Hilkka Timonen
Atmos. Chem. Phys., 23, 2963–2982, https://doi.org/10.5194/acp-23-2963-2023, https://doi.org/10.5194/acp-23-2963-2023, 2023
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This study elucidates properties and sources of volatile organic compounds (VOCs) and organic aerosol (OA) in a traffic environment. Anthropogenic VOCs (aVOCs) were clearly higher than biogenic VOCs (bVOCs), but bVOCs produced a larger portion of oxidation products. OA consisted mostly of oxygenated OA, representing secondary OA (SOA). SOA was partly associated with bVOCs, but it was also related to long-range transport. Primary OA originated mostly from traffic.
Detlev Helmig, Alex Guenther, Jacques Hueber, Ryan Daly, Wei Wang, Jeong-Hoo Park, Anssi Liikanen, and Arnaud P. Praplan
Atmos. Meas. Tech., 15, 5439–5454, https://doi.org/10.5194/amt-15-5439-2022, https://doi.org/10.5194/amt-15-5439-2022, 2022
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This research demonstrates a new method for determination of the chemical reactivity of volatile organic compounds that are emitted from the leaves and needles of trees. These measurements allow elucidating if and how much of these emissions and their associated reactivity are captured and quantified by currently applicable chemical analysis methods.
Hannele Hakola, Ditte Taipale, Arnaud Praplan, Simon Schallhart, Steven Thomas, Toni Tykkä, Aku Helin, Jaana Bäck, and Heidi Hellén
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-478, https://doi.org/10.5194/acp-2022-478, 2022
Revised manuscript not accepted
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Norway spruce is one of the main tree species growing in the boreal area. We show that volatile organic compound emission potentials and compound composition vary a lot. We have investigated if e.g. growing location or age of a tree could explain the variations. Recognizing this observed large variability in spruce BVOC emissions (precursors for new particle formation processes), we also tested the consequences of this variability in simulations of aerosol formation.
Niel Verbrigghe, Niki I. W. Leblans, Bjarni D. Sigurdsson, Sara Vicca, Chao Fang, Lucia Fuchslueger, Jennifer L. Soong, James T. Weedon, Christopher Poeplau, Cristina Ariza-Carricondo, Michael Bahn, Bertrand Guenet, Per Gundersen, Gunnhildur E. Gunnarsdóttir, Thomas Kätterer, Zhanfeng Liu, Marja Maljanen, Sara Marañón-Jiménez, Kathiravan Meeran, Edda S. Oddsdóttir, Ivika Ostonen, Josep Peñuelas, Andreas Richter, Jordi Sardans, Páll Sigurðsson, Margaret S. Torn, Peter M. Van Bodegom, Erik Verbruggen, Tom W. N. Walker, Håkan Wallander, and Ivan A. Janssens
Biogeosciences, 19, 3381–3393, https://doi.org/10.5194/bg-19-3381-2022, https://doi.org/10.5194/bg-19-3381-2022, 2022
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In subarctic grassland on a geothermal warming gradient, we found large reductions in topsoil carbon stocks, with carbon stocks linearly declining with warming intensity. Most importantly, however, we observed that soil carbon stocks stabilised within 5 years of warming and remained unaffected by warming thereafter, even after > 50 years of warming. Moreover, in contrast to the large topsoil carbon losses, subsoil carbon stocks remained unaffected after > 50 years of soil warming.
Lisa J. Beck, Siegfried Schobesberger, Heikki Junninen, Janne Lampilahti, Antti Manninen, Lubna Dada, Katri Leino, Xu-Cheng He, Iida Pullinen, Lauriane L. J. Quéléver, Anna Franck, Pyry Poutanen, Daniela Wimmer, Frans Korhonen, Mikko Sipilä, Mikael Ehn, Douglas R. Worsnop, Veli-Matti Kerminen, Tuukka Petäjä, Markku Kulmala, and Jonathan Duplissy
Atmos. Chem. Phys., 22, 8547–8577, https://doi.org/10.5194/acp-22-8547-2022, https://doi.org/10.5194/acp-22-8547-2022, 2022
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The presented article introduces an overview of atmospheric ions and their composition above the boreal forest. We provide the results of an extensive airborne measurement campaign with an air ion mass spectrometer and particle measurements, showing their diurnal evolution within the boundary layer and free troposphere. In addition, we compare the airborne dataset with the co-located data from the ground at SMEAR II station, Finland.
Haiyan Li, Thomas Golin Almeida, Yuanyuan Luo, Jian Zhao, Brett B. Palm, Christopher D. Daub, Wei Huang, Claudia Mohr, Jordan E. Krechmer, Theo Kurtén, and Mikael Ehn
Atmos. Meas. Tech., 15, 1811–1827, https://doi.org/10.5194/amt-15-1811-2022, https://doi.org/10.5194/amt-15-1811-2022, 2022
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This work evaluated the potential for PTR-based mass spectrometers to detect ROOR and ROOH peroxides both experimentally and through computations. Laboratory experiments using a Vocus PTR observed only noisy signals of potential dimers during α-pinene ozonolysis and a few small signals of dimeric compounds during cyclohexene ozonolysis. Quantum chemical calculations for model ROOR and ROOH systems showed that most of these peroxides should fragment partially following protonation.
Timo Vesala, Kukka-Maaria Kohonen, Linda M. J. Kooijmans, Arnaud P. Praplan, Lenka Foltýnová, Pasi Kolari, Markku Kulmala, Jaana Bäck, David Nelson, Dan Yakir, Mark Zahniser, and Ivan Mammarella
Atmos. Chem. Phys., 22, 2569–2584, https://doi.org/10.5194/acp-22-2569-2022, https://doi.org/10.5194/acp-22-2569-2022, 2022
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Carbonyl sulfide (COS) provides new insights into carbon cycle research. We present an easy-to-use flux parameterization and the longest existing time series of forest–atmosphere COS exchange measurements, which allow us to study both seasonal and interannual variability. We observed only uptake of COS by the forest on an annual basis, with 37 % variability between years. Upscaling the boreal COS uptake using a biosphere model indicates a significant missing COS sink at high latitudes.
Lore T. Verryckt, Sara Vicca, Leandro Van Langenhove, Clément Stahl, Dolores Asensio, Ifigenia Urbina, Romà Ogaya, Joan Llusià, Oriol Grau, Guille Peguero, Albert Gargallo-Garriga, Elodie A. Courtois, Olga Margalef, Miguel Portillo-Estrada, Philippe Ciais, Michael Obersteiner, Lucia Fuchslueger, Laynara F. Lugli, Pere-Roc Fernandez-Garberí, Helena Vallicrosa, Melanie Verlinden, Christian Ranits, Pieter Vermeir, Sabrina Coste, Erik Verbruggen, Laëtitia Bréchet, Jordi Sardans, Jérôme Chave, Josep Peñuelas, and Ivan A. Janssens
Earth Syst. Sci. Data, 14, 5–18, https://doi.org/10.5194/essd-14-5-2022, https://doi.org/10.5194/essd-14-5-2022, 2022
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We provide a comprehensive dataset of vertical profiles of photosynthesis and important leaf traits, including leaf N and P concentrations, from two 3-year, large-scale nutrient addition experiments conducted in two tropical rainforests in French Guiana. These data present a unique source of information to further improve model representations of the roles of N and P, and other leaf nutrients, in photosynthesis in tropical forests.
Ditte Taipale, Veli-Matti Kerminen, Mikael Ehn, Markku Kulmala, and Ülo Niinemets
Atmos. Chem. Phys., 21, 17389–17431, https://doi.org/10.5194/acp-21-17389-2021, https://doi.org/10.5194/acp-21-17389-2021, 2021
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Larval feeding and fungal infections of leaves can greatly change the emission of volatile compounds from plants and thereby influence aerosol processes in the air. We developed a model that considers the dynamics of larvae and fungi and the dependency of the emission on the severity of stress. We show that the infections can be highly atmospherically relevant during long periods of time and at times more important to consider than the parameters that are currently used in emission models.
Yuliang Liu, Wei Nie, Yuanyuan Li, Dafeng Ge, Chong Liu, Zhengning Xu, Liangduo Chen, Tianyi Wang, Lei Wang, Peng Sun, Ximeng Qi, Jiaping Wang, Zheng Xu, Jian Yuan, Chao Yan, Yanjun Zhang, Dandan Huang, Zhe Wang, Neil M. Donahue, Douglas Worsnop, Xuguang Chi, Mikael Ehn, and Aijun Ding
Atmos. Chem. Phys., 21, 14789–14814, https://doi.org/10.5194/acp-21-14789-2021, https://doi.org/10.5194/acp-21-14789-2021, 2021
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Oxygenated organic molecules (OOMs) are crucial intermediates linking volatile organic compounds to secondary organic aerosols. Using nitrate time-of-flight chemical ionization mass spectrometry in eastern China, we performed positive matrix factorization (PMF) on binned OOM mass spectra. We reconstructed over 1000 molecules from 14 derived PMF factors and identified about 72 % of the observed OOMs as organic nitrates, highlighting the decisive role of NOx in OOM formation in populated areas.
Janne Lampilahti, Hanna E. Manninen, Tuomo Nieminen, Sander Mirme, Mikael Ehn, Iida Pullinen, Katri Leino, Siegfried Schobesberger, Juha Kangasluoma, Jenni Kontkanen, Emma Järvinen, Riikka Väänänen, Taina Yli-Juuti, Radovan Krejci, Katrianne Lehtipalo, Janne Levula, Aadu Mirme, Stefano Decesari, Ralf Tillmann, Douglas R. Worsnop, Franz Rohrer, Astrid Kiendler-Scharr, Tuukka Petäjä, Veli-Matti Kerminen, Thomas F. Mentel, and Markku Kulmala
Atmos. Chem. Phys., 21, 12649–12663, https://doi.org/10.5194/acp-21-12649-2021, https://doi.org/10.5194/acp-21-12649-2021, 2021
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We studied aerosol particle formation and growth in different parts of the planetary boundary layer at two different locations (Po Valley, Italy, and Hyytiälä, Finland). The observations consist of airborne measurements on board an instrumented Zeppelin and a small airplane combined with comprehensive ground-based measurements.
Louise N. Jensen, Manjula R. Canagaratna, Kasper Kristensen, Lauriane L. J. Quéléver, Bernadette Rosati, Ricky Teiwes, Marianne Glasius, Henrik B. Pedersen, Mikael Ehn, and Merete Bilde
Atmos. Chem. Phys., 21, 11545–11562, https://doi.org/10.5194/acp-21-11545-2021, https://doi.org/10.5194/acp-21-11545-2021, 2021
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This work targets the chemical composition of α-pinene-derived secondary organic aerosol (SOA) formed in the temperature range from -15 to 20°C. Experiments were conducted in an atmospheric simulation chamber. Positive matrix factorization analysis of data obtained by a high-resolution time-of-flight aerosol mass spectrometer shows that the elemental aerosol composition is controlled by the initial α-pinene concentration and temperature during SOA formation.
Liine Heikkinen, Mikko Äijälä, Kaspar R. Daellenbach, Gang Chen, Olga Garmash, Diego Aliaga, Frans Graeffe, Meri Räty, Krista Luoma, Pasi Aalto, Markku Kulmala, Tuukka Petäjä, Douglas Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 21, 10081–10109, https://doi.org/10.5194/acp-21-10081-2021, https://doi.org/10.5194/acp-21-10081-2021, 2021
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In many locations worldwide aerosol particles have been shown to be made up of organic aerosol (OA). The boreal forest is a region where aerosol particles possess a high OA mass fraction. Here, we studied OA composition using the longest time series of OA composition ever obtained from a boreal environment. For this purpose, we tested a new analysis framework and discovered that most of the OA was highly oxidized, with strong seasonal behaviour reflecting different sources in summer and winter.
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.
Heidi Hellén, Arnaud P. Praplan, Toni Tykkä, Aku Helin, Simon Schallhart, Piia P. Schiestl-Aalto, Jaana Bäck, and Hannele Hakola
Atmos. Chem. Phys., 21, 8045–8066, https://doi.org/10.5194/acp-21-8045-2021, https://doi.org/10.5194/acp-21-8045-2021, 2021
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Even though terpene emissions of boreal needle trees have been studied quite intensively, there is less knowledge of the emissions of broadleaved deciduous trees and emissions of larger terpenes and oxygenated volatile organic compounds. Here we studied downy birch (Betula pubescens) emissions, and especially sesquiterpene and oxygenated sesquiterpene emissions were found to be high. These emissions may have significant effects on secondary organic aerosol formation in boreal areas.
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.
Runlong Cai, Yihao Li, Yohann Clément, Dandan Li, Clément Dubois, Marlène Fabre, Laurence Besson, Sebastien Perrier, Christian George, Mikael Ehn, Cheng Huang, Ping Yi, Yingge Ma, and Matthieu Riva
Atmos. Meas. Tech., 14, 2377–2387, https://doi.org/10.5194/amt-14-2377-2021, https://doi.org/10.5194/amt-14-2377-2021, 2021
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Orbitool is an open-source software tool, mainly coded in Python, with a graphical user interface (GUI), specifically developed to facilitate the analysis of online Orbitrap mass spectrometric data. It is notably optimized for long-term atmospheric measurements and laboratory studies.
Haiyan Li, Manjula R. Canagaratna, Matthieu Riva, Pekka Rantala, Yanjun Zhang, Steven Thomas, Liine Heikkinen, Pierre-Marie Flaud, Eric Villenave, Emilie Perraudin, Douglas Worsnop, Markku Kulmala, Mikael Ehn, and Federico Bianchi
Atmos. Chem. Phys., 21, 4123–4147, https://doi.org/10.5194/acp-21-4123-2021, https://doi.org/10.5194/acp-21-4123-2021, 2021
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For the first time, we performed binPMF analysis on the complex mass spectra acquired with the Vocus PTR-TOF in two European pine forests and identified various primary emission sources and secondary oxidation processes of atmospheric organic vapors, i.e., terpenes and their oxidation products, with varying oxidation degrees. Further insights were gained regarding monoterpene and sesquiterpene reactions based on the interpretation results.
Michael Priestley, Thomas J. Bannan, Michael Le Breton, Stephen D. Worrall, Sungah Kang, Iida Pullinen, Sebastian Schmitt, Ralf Tillmann, Einhard Kleist, Defeng Zhao, Jürgen Wildt, Olga Garmash, Archit Mehra, Asan Bacak, Dudley E. Shallcross, Astrid Kiendler-Scharr, Åsa M. Hallquist, Mikael Ehn, Hugh Coe, Carl J. Percival, Mattias Hallquist, Thomas F. Mentel, and Gordon McFiggans
Atmos. Chem. Phys., 21, 3473–3490, https://doi.org/10.5194/acp-21-3473-2021, https://doi.org/10.5194/acp-21-3473-2021, 2021
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A significant fraction of emissions from human activity consists of aromatic hydrocarbons, e.g. benzene, which oxidise to form new compounds important for particle growth. Characterisation of benzene oxidation products highlights the range of species produced as well as their chemical properties and contextualises them within relevant frameworks, e.g. MCM. Cluster analysis of the oxidation product time series distinguishes behaviours of CHON compounds that could aid in identifying functionality.
Kasper Kristensen, Louise N. Jensen, Lauriane L. J. Quéléver, Sigurd Christiansen, Bernadette Rosati, Jonas Elm, Ricky Teiwes, Henrik B. Pedersen, Marianne Glasius, Mikael Ehn, and Merete Bilde
Atmos. Chem. Phys., 20, 12549–12567, https://doi.org/10.5194/acp-20-12549-2020, https://doi.org/10.5194/acp-20-12549-2020, 2020
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Atmospheric particles are important in relation to human health and the global climate. As the global temperature changes, so may the atmospheric chemistry controlling the formation of particles from reactions of naturally emitted volatile organic compounds (VOCs). In the current work, we show how temperatures influence the formation and chemical composition of atmospheric particles from α-pinene: a biogenic VOC largely emitted in high-latitude environments such as the boreal forests.
Arnaud P. Praplan, Toni Tykkä, Simon Schallhart, Virpi Tarvainen, Jaana Bäck, and Heidi Hellén
Biogeosciences, 17, 4681–4705, https://doi.org/10.5194/bg-17-4681-2020, https://doi.org/10.5194/bg-17-4681-2020, 2020
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In this paper, we study emissions of volatile organic compounds (VOCs) from three boreal tree species. Individual compounds are quantified with on-line separation analytical techniques, while the total reactivity of the emissions is measured using a custom-built instrument. On some occasions, in particular when the trees suffer from stress, the total reactivity measured is higher than the sum of the reactivity of individual compounds. This indicates that the threes emit VOCs that remain unknown.
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Short summary
Diterpenes were only recently observed in the atmosphere, and little is known of their atmospheric fates. We explored the ozonolysis of the diterpene kaurene in a chamber, and we characterized the oxidation products for the first time using chemical ionization mass spectrometry. Our findings highlight similarities and differences between diterpenes and smaller terpenes during their atmospheric oxidation.
Diterpenes were only recently observed in the atmosphere, and little is known of their...
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