Articles | Volume 20, issue 21
https://doi.org/10.5194/acp-20-12549-2020
© Author(s) 2020. 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-20-12549-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| Highlight paper
| 
02 Nov 2020
Research article | Highlight paper |
| 02 Nov 2020
| 02 Nov 2020
The Aarhus Chamber Campaign on Highly Oxygenated Organic Molecules and Aerosols (ACCHA): particle formation, organic acids, and dimer esters from α-pinene ozonolysis at different temperatures
Kasper Kristensen
CORRESPONDING AUTHOR
Department of Engineering, Aarhus University, 8000 Aarhus C, Denmark
Louise N. Jensen
Department of Chemistry and iCLIMATE, Aarhus University, 8000 Aarhus
C, Denmark
Lauriane L. J. Quéléver
Institute for Atmospheric and Earth System Research – INAR/Physics,
University of Helsinki, P.O. Box 64, 00014, Helsinki, Finland
Sigurd Christiansen
Department of Chemistry and iCLIMATE, Aarhus University, 8000 Aarhus
C, Denmark
Bernadette Rosati
Department of Chemistry and iCLIMATE, Aarhus University, 8000 Aarhus
C, Denmark
Department of Physics and Astronomy, Aarhus University, 8000 Aarhus C,
Denmark
Jonas Elm
Department of Chemistry and iCLIMATE, Aarhus University, 8000 Aarhus
C, Denmark
Ricky Teiwes
Department of Physics and Astronomy, Aarhus University, 8000 Aarhus C,
Denmark
Henrik B. Pedersen
Department of Physics and Astronomy, Aarhus University, 8000 Aarhus C,
Denmark
Marianne Glasius
Department of Chemistry and iCLIMATE, Aarhus University, 8000 Aarhus
C, Denmark
Mikael Ehn
Institute for Atmospheric and Earth System Research – INAR/Physics,
University of Helsinki, P.O. Box 64, 00014, Helsinki, Finland
Department of Chemistry and iCLIMATE, Aarhus University, 8000 Aarhus
C, Denmark
Related authors
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
Short summary
Short summary
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.
Maija Peltola, Roseline Thakur, Kurt Spence, Janne Lampilahti, Ronja Mäkelä, Sasu Karttunen, Ekaterina Ezhova, Sami Haapanala, Aki Vähä, Juha Kangasluoma, Tommy Chan, Pauli Paasonen, Joanna Norkko, Alf Norkko, Markku Kulmala, and Mikael Ehn
EGUsphere, https://doi.org/10.5194/egusphere-2025-3809, https://doi.org/10.5194/egusphere-2025-3809, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
Short summary
Short summary
Here we report aerosol properties from a new atmospheric observatory established at the Finnish Baltic Sea Coast. Aerosol formation was observed when air masses crossed over the continent whereas less newly formed particles were observed when the winds were from the sea. Aerosol formation was favoured by low condensation sink and sunny dry conditions.
Neil M. Donahue, Victoria Hofbauer, Henning Finkenzeller, Dominik Stolzenburg, Paulus S. Bauer, Randall Chiu, Lubna Dada, Jonathan Duplissy, Xu-Cheng He, Martin Heinritzi, Christopher R. Hoyle, Andreas Kürten, Aleksandr Kvashnin, Katrianne Lehtipalo, Naser Mahfouz, Vladimir Makhmutov, Roy L. Mauldin III, Ugo Molteni, Lauriane L. J. Quéléver, Matti Rissanen, Siegfried Schobesberger, Mario Simon, Andrea C. Wagner, Mingyi Wang, Chao Yan, Penglin Ye, Ilona Riipinen, Hamish Gordon, Joachim Curtius, Armin Hansel, Imad El Haddad, Markku Kulmala, Douglas R. Worsnop, Rainer Volkamer, Paul M. Winkler, Jasper Kirkby, and Richard Flagan
EGUsphere, https://doi.org/10.5194/egusphere-2025-2412, https://doi.org/10.5194/egusphere-2025-2412, 2025
This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
Short summary
Short summary
We describe accurate measurement of particle formation and growth in the CERN CLOUD chamber, using a suite of gas- and particle-phase instruments. The interconnected measurements establish high accuracy in key particle properties and critically important gas-phase sulfuric acid. This is a template for accurate calibration of similar experiments and thus accurate determination of aerosol nucleation and growth rates, which are an important source of uncertainty in climate science.
Yosef Knattrup, Ivo Neefjes, Jakub Kubečka, and Jonas Elm
Aerosol Research, 3, 237–251, https://doi.org/10.5194/ar-3-237-2025, https://doi.org/10.5194/ar-3-237-2025, 2025
Short summary
Short summary
Aerosols, a large uncertainty in climate modeling, can be formed when gas vapors and particles begin sticking together. Traditionally, these particles are assumed to behave like hard spheres that only stick together upon head-on collisions. In reality, particles can attract each other over distances, leading to more frequent sticking events. We found that traditional models significantly undercount these events, with real sticking rates being up to 2.4 times higher.
Yuanyuan Luo, Lauri Franzon, Jiangyi Zhang, Nina Sarnela, Neil M. Donahue, Theo Kurtén, and Mikael Ehn
Atmos. Chem. Phys., 25, 4655–4664, https://doi.org/10.5194/acp-25-4655-2025, https://doi.org/10.5194/acp-25-4655-2025, 2025
Short summary
Short summary
This study explores the formation of accretion products from reactions involving highly reactive compounds, Criegee intermediates. We focused on three types of terpenes, common in nature, and their reactions with specific acids. Our findings reveal that these reactions efficiently produce expected compounds. This research enhances our understanding of how these reactions affect air quality and climate by contributing to aerosol formation, crucial for atmospheric chemistry.
Valter Mickwitz, Otso Peräkylä, Frans Graeffe, Douglas Worsnop, and Mikael Ehn
Atmos. Meas. Tech., 18, 1537–1559, https://doi.org/10.5194/amt-18-1537-2025, https://doi.org/10.5194/amt-18-1537-2025, 2025
Short summary
Short summary
This work presents and evaluates an algorithm that automatically conducts the steps of fitting peaks and identifying formulas – necessary but time-consuming steps for most applications of mass spectrometry in atmospheric science. The aim of the algorithm is to save researchers working on these tasks significant amounts of time and allow them to proceed with their analysis. The work demonstrates that this algorithm can achieve the goal of speeding up analysis and provide accurate formulas.
Frans Graeffe, Kalle Kupi, Hilkka Timonen, and Mikael Ehn
EGUsphere, https://doi.org/10.5194/egusphere-2025-910, https://doi.org/10.5194/egusphere-2025-910, 2025
Short summary
Short summary
Alkanes are a major part of anthropogenic emissions in urban areas, and known for being capable of producing secondary organic aerosol (SOA). We measured SOA yields of seven alkanes and their oxygenated derivatives in oxidation flow reactor measurements to assess their role in SOA formation. In addition to quantified SOA yields, we observed that cyclic structure enhances SOA production. Furthermore, our observations indicate that multi-generational OH oxidation is important in the SOA formation.
Hector Navarro-Barboza, Jordi Rovira, Vincenzo Obiso, Andrea Pozzer, Marta Via, Andres Alastuey, Xavier Querol, Noemi Perez, Marjan Savadkoohi, Gang Chen, Jesus Yus-Díez, Matic Ivancic, Martin Rigler, Konstantinos Eleftheriadis, Stergios Vratolis, Olga Zografou, Maria Gini, Benjamin Chazeau, Nicolas Marchand, Andre S. H. Prevot, Kaspar Dallenbach, Mikael Ehn, Krista Luoma, Tuukka Petäjä, Anna Tobler, Jaroslaw Necki, Minna Aurela, Hilkka Timonen, Jarkko Niemi, Olivier Favez, Jean-Eudes Petit, Jean-Philippe Putaud, Christoph Hueglin, Nicolas Pascal, Aurélien Chauvigné, Sébastien Conil, Marco Pandolfi, and Oriol Jorba
Atmos. Chem. Phys., 25, 2667–2694, https://doi.org/10.5194/acp-25-2667-2025, https://doi.org/10.5194/acp-25-2667-2025, 2025
Short summary
Short summary
Brown carbon (BrC) absorbs ultraviolet (UV) and visible light, influencing climate. This study explores BrC's imaginary refractive index (k) using data from 12 European sites. Residential emissions are a major organic aerosol (OA) source in winter, while secondary organic aerosol (SOA) dominates in summer. Source-specific k values were derived, improving model accuracy. The findings highlight BrC's climate impact and emphasize source-specific constraints in atmospheric models.
Yosef Knattrup and Jonas Elm
Aerosol Research, 3, 125–137, https://doi.org/10.5194/ar-3-125-2025, https://doi.org/10.5194/ar-3-125-2025, 2025
Short summary
Short summary
Using quantum chemical methods, we studied the uptake of first-generation oxidation products onto freshly nucleated particles (FNPs). We find that pinic acid can condense on these small FNPs at realistic atmospheric conditions, thereby contributing to early particle growth. The mechanism involves two pinic acid molecules interacting with each other, showing that direct organic–organic interactions during co-condensation onto the particle contribute to the growth.
Galib Hasan, Haide Wu, Yosef Knattrup, and Jonas Elm
Aerosol Research, 3, 101–111, https://doi.org/10.5194/ar-3-101-2025, https://doi.org/10.5194/ar-3-101-2025, 2025
Short summary
Short summary
Aerosol formation is an important process for our global climate. However, there are high uncertainties associated with the formation of new aerosol particles. We present quantum chemical calculations of large atmospheric molecular clusters composed of sulfuric acid (SA), ammonia (AM), and dimethylamine (DMA). We find that mixed SA–AM–DMA systems cluster more efficiently for freshly nucleated particles compared to pure SA–AM and SA–DMA systems.
Benjamin Heutte, Nora Bergner, Hélène Angot, Jakob B. Pernov, Lubna Dada, Jessica A. Mirrielees, Ivo Beck, Andrea Baccarini, Matthew Boyer, Jessie M. Creamean, Kaspar R. Daellenbach, Imad El Haddad, Markus M. Frey, Silvia Henning, Tiia Laurila, Vaios Moschos, Tuukka Petäjä, Kerri A. Pratt, Lauriane L. J. Quéléver, Matthew D. Shupe, Paul Zieger, Tuija Jokinen, and Julia Schmale
Atmos. Chem. Phys., 25, 2207–2241, https://doi.org/10.5194/acp-25-2207-2025, https://doi.org/10.5194/acp-25-2207-2025, 2025
Short summary
Short summary
Limited aerosol measurements in the central Arctic hinder our understanding of aerosol–climate interactions in the region. Our year-long observations of aerosol physicochemical properties during the MOSAiC expedition reveal strong seasonal variations in aerosol chemical composition, where the short-term variability is heavily affected by storms in the Arctic. Local wind-generated particles are shown to be an important source of cloud seeds, especially in autumn.
James Brean, David C. S. Beddows, Eija Asmi, Aki Virkkula, Lauriane L. J. Quéléver, Mikko Sipilä, Floortje Van Den Heuvel, Thomas Lachlan-Cope, Anna Jones, Markus Frey, Angelo Lupi, Jiyeon Park, Young Jun Yoon, Rolf Weller, Giselle L. Marincovich, Gabriela C. Mulena, Roy M. Harrison, and Manuel Dall'Osto
Atmos. Chem. Phys., 25, 1145–1162, https://doi.org/10.5194/acp-25-1145-2025, https://doi.org/10.5194/acp-25-1145-2025, 2025
Short summary
Short summary
Our results emphasise how understanding the geographical variation in surface types across the Antarctic is key to understanding secondary aerosol sources.
Haide Wu, Yosef Knattrup, Andreas Buchgraitz Jensen, and Jonas Elm
Aerosol Research, 2, 303–314, https://doi.org/10.5194/ar-2-303-2024, https://doi.org/10.5194/ar-2-303-2024, 2024
Short summary
Short summary
The exact point at which a given assembly of molecules represents an atmospheric molecular cluster or a particle remains ambiguous. Using quantum chemical methods, here we explore a cluster-to-particle transition point. Based on our results, we deduce a property-based criterion for defining freshly nucleated particles (FNPs) that act as a boundary between discrete cluster configurations and bulk particles.
Matthew Boyer, Diego Aliaga, Lauriane L. J. Quéléver, Silvia Bucci, Hélène Angot, Lubna Dada, Benjamin Heutte, Lisa Beck, Marina Duetsch, Andreas Stohl, Ivo Beck, Tiia Laurila, Nina Sarnela, Roseline C. Thakur, Branka Miljevic, Markku Kulmala, Tuukka Petäjä, Mikko Sipilä, Julia Schmale, and Tuija Jokinen
Atmos. Chem. Phys., 24, 12595–12621, https://doi.org/10.5194/acp-24-12595-2024, https://doi.org/10.5194/acp-24-12595-2024, 2024
Short summary
Short summary
We analyze the seasonal cycle and sources of gases that are relevant for the formation of aerosol particles in the central Arctic. Since theses gases can form new particles, they can influence Arctic climate. We show that the sources of these gases are associated with changes in the Arctic environment during the year, especially with respect to sea ice. Therefore, the concentration of these gases will likely change in the future as the Arctic continues to warm.
Yuanyuan Luo, Ditte Thomsen, Emil Mark Iversen, Pontus Roldin, Jane Tygesen Skønager, Linjie Li, Michael Priestley, Henrik B. Pedersen, Mattias Hallquist, Merete Bilde, Marianne Glasius, and Mikael Ehn
Atmos. Chem. Phys., 24, 9459–9473, https://doi.org/10.5194/acp-24-9459-2024, https://doi.org/10.5194/acp-24-9459-2024, 2024
Short summary
Short summary
∆3-carene is abundantly emitted from vegetation, but its atmospheric oxidation chemistry has received limited attention. We explored highly oxygenated organic molecule (HOM) formation from ∆3-carene ozonolysis in chambers and investigated the impact of temperature and relative humidity on HOM formation. Our findings provide new insights into ∆3-carene oxidation pathways and their potential to impact atmospheric aerosols.
Astrid Nørskov Pedersen, Yosef Knattrup, and Jonas Elm
Aerosol Research, 2, 123–134, https://doi.org/10.5194/ar-2-123-2024, https://doi.org/10.5194/ar-2-123-2024, 2024
Short summary
Short summary
Aerosol formation is an important process for our global climate. While inorganic species have been shown to be important for aerosol formation, there remains a large gap in our knowledge about the exact involvement of organics. We present a new quantum chemical procedure for screening relevant organics that for the first time allows us to obtain direct molecular-level insight into the organics involved in aerosol formation.
Jian Zhao, Valter Mickwitz, Yuanyuan Luo, Ella Häkkinen, Frans Graeffe, Jiangyi Zhang, Hilkka Timonen, Manjula Canagaratna, Jordan E. Krechmer, Qi Zhang, Markku Kulmala, Juha Kangasluoma, Douglas Worsnop, and Mikael Ehn
Atmos. Meas. Tech., 17, 1527–1543, https://doi.org/10.5194/amt-17-1527-2024, https://doi.org/10.5194/amt-17-1527-2024, 2024
Short summary
Short summary
Organic aerosol constitutes a significant portion of atmospheric fine particles but is less characterized due to its vast number of constituents. Recently, we developed a system for online measurements of particle-phase highly oxygenated organic molecules (HOMs). In this work, we systematically characterized the system, developed a new unit to enhance its performance, and demonstrated the essential role of thermograms in inferring volatility and quantifying HOMs in organic aerosols.
Jiangyi Zhang, Jian Zhao, Yuanyuan Luo, Valter Mickwitz, Douglas Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 24, 2885–2911, https://doi.org/10.5194/acp-24-2885-2024, https://doi.org/10.5194/acp-24-2885-2024, 2024
Short summary
Short summary
Due to the intrinsic connection between the formation pathways of O3 and HOMs, the ratio of HOM dimers or non-nitrate monomers to HOM organic nitrates could be used to determine O3 formation regimes. Owing to the fast formation and short lifetimes of HOMs, HOM-based indicating ratios can describe O3 formation in real time. Despite the success of our approach in this simple laboratory system, applicability to the much more complex atmosphere remains to be determined.
Jing Cai, Juha Sulo, Yifang Gu, Sebastian Holm, Runlong Cai, Steven Thomas, Almuth Neuberger, Fredrik Mattsson, Marco Paglione, Stefano Decesari, Matteo Rinaldi, Rujing Yin, Diego Aliaga, Wei Huang, Yuanyuan Li, Yvette Gramlich, Giancarlo Ciarelli, Lauriane Quéléver, Nina Sarnela, Katrianne Lehtipalo, Nora Zannoni, Cheng Wu, Wei Nie, Juha Kangasluoma, Claudia Mohr, Markku Kulmala, Qiaozhi Zha, Dominik Stolzenburg, and Federico Bianchi
Atmos. Chem. Phys., 24, 2423–2441, https://doi.org/10.5194/acp-24-2423-2024, https://doi.org/10.5194/acp-24-2423-2024, 2024
Short summary
Short summary
By combining field measurements, simulations and recent chamber experiments, we investigate new particle formation (NPF) and growth in the Po Valley, where both haze and frequent NPF occur. Our results show that sulfuric acid, ammonia and amines are the dominant NPF precursors there. A high NPF rate and a lower condensation sink lead to a greater survival probability for newly formed particles, highlighting the importance of gas-to-particle conversion for aerosol concentrations.
Magdalena Okuljar, Olga Garmash, Miska Olin, Joni Kalliokoski, Hilkka Timonen, Jarkko V. Niemi, Pauli Paasonen, Jenni Kontkanen, Yanjun Zhang, Heidi Hellén, Heino Kuuluvainen, Minna Aurela, Hanna E. Manninen, Mikko Sipilä, Topi Rönkkö, Tuukka Petäjä, Markku Kulmala, Miikka Dal Maso, and Mikael Ehn
Atmos. Chem. Phys., 23, 12965–12983, https://doi.org/10.5194/acp-23-12965-2023, https://doi.org/10.5194/acp-23-12965-2023, 2023
Short summary
Short summary
Highly oxygenated organic molecules (HOMs) form secondary organic aerosol that affects air quality and health. In this study, we demonstrate that in a moderately polluted city with abundant vegetation, the composition of HOMs is largely controlled by the effect of NOx on the biogenic volatile organic compound oxidation. Comparing the results from two nearby stations, we show that HOM composition and formation pathways can change considerably within small distances in urban environments.
Dimitri Castarède, Zoé Brasseur, Yusheng Wu, Zamin A. Kanji, Markus Hartmann, Lauri Ahonen, Merete Bilde, Markku Kulmala, Tuukka Petäjä, Jan B. C. Pettersson, Berko Sierau, Olaf Stetzer, Frank Stratmann, Birgitta Svenningsson, Erik Swietlicki, Quynh Thu Nguyen, Jonathan Duplissy, and Erik S. Thomson
Atmos. Meas. Tech., 16, 3881–3899, https://doi.org/10.5194/amt-16-3881-2023, https://doi.org/10.5194/amt-16-3881-2023, 2023
Short summary
Short summary
Clouds play a key role in Earth’s climate by influencing the surface energy budget. Certain types of atmospheric aerosols, called ice-nucleating particles (INPs), induce the formation of ice in clouds and, thus, often initiate precipitation formation. The Portable Ice Nucleation Chamber 2 (PINCii) is a new instrument developed to study ice formation and to conduct ambient measurements of INPs, allowing us to investigate the sources and properties of the atmospheric aerosols that can act as INPs.
Jonas Elm, Aladár Czitrovszky, Andreas Held, Annele Virtanen, Astrid Kiendler-Scharr, Benjamin J. Murray, Daniel McCluskey, Daniele Contini, David Broday, Eirini Goudeli, Hilkka Timonen, Joan Rosell-Llompart, Jose L. Castillo, Evangelia Diapouli, Mar Viana, Maria E. Messing, Markku Kulmala, Naděžda Zíková, and Sebastian H. Schmitt
Aerosol Research, 1, 13–16, https://doi.org/10.5194/ar-1-13-2023, https://doi.org/10.5194/ar-1-13-2023, 2023
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
Short summary
Short summary
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.
Ella Häkkinen, Jian Zhao, Frans Graeffe, Nicolas Fauré, Jordan E. Krechmer, Douglas Worsnop, Hilkka Timonen, Mikael Ehn, and Juha Kangasluoma
Atmos. Meas. Tech., 16, 1705–1721, https://doi.org/10.5194/amt-16-1705-2023, https://doi.org/10.5194/amt-16-1705-2023, 2023
Short summary
Short summary
Highly oxygenated compounds contribute to the formation and growth of atmospheric organic aerosol and thus impact the global climate. Knowledge of their transformations and fate after condensing into the particle phase has been limited by the lack of suitable detection techniques. Here, we present an online method for measuring highly oxygenated compounds from organic aerosol. We evaluate the performance of the method and demonstrate that the method is applicable to different organic species.
Jian Zhao, Ella Häkkinen, Frans Graeffe, Jordan E. Krechmer, Manjula R. Canagaratna, Douglas R. Worsnop, Juha Kangasluoma, and Mikael Ehn
Atmos. Chem. Phys., 23, 3707–3730, https://doi.org/10.5194/acp-23-3707-2023, https://doi.org/10.5194/acp-23-3707-2023, 2023
Short summary
Short summary
Based on the combined measurements of gas- and particle-phase highly oxygenated organic molecules (HOMs) from α-pinene ozonolysis, enhancement of dimers in particles was observed. We conducted experiments wherein the dimer to monomer (D / M) ratios of HOMs in the gas phase were modified (adding CO / NO) to investigate the effects of the corresponding D / M ratios in the particles. These results are important for a better understanding of secondary organic aerosol formation in the atmosphere.
Matthew Boyer, Diego Aliaga, Jakob Boyd Pernov, Hélène Angot, Lauriane L. J. Quéléver, Lubna Dada, Benjamin Heutte, Manuel Dall'Osto, David C. S. Beddows, Zoé Brasseur, Ivo Beck, Silvia Bucci, Marina Duetsch, Andreas Stohl, Tiia Laurila, Eija Asmi, Andreas Massling, Daniel Charles Thomas, Jakob Klenø Nøjgaard, Tak Chan, Sangeeta Sharma, Peter Tunved, Radovan Krejci, Hans Christen Hansson, Federico Bianchi, Katrianne Lehtipalo, Alfred Wiedensohler, Kay Weinhold, Markku Kulmala, Tuukka Petäjä, Mikko Sipilä, Julia Schmale, and Tuija Jokinen
Atmos. Chem. Phys., 23, 389–415, https://doi.org/10.5194/acp-23-389-2023, https://doi.org/10.5194/acp-23-389-2023, 2023
Short summary
Short summary
The Arctic is a unique environment that is warming faster than other locations on Earth. We evaluate measurements of aerosol particles, which can influence climate, over the central Arctic Ocean for a full year and compare the data to land-based measurement stations across the Arctic. Our measurements show that the central Arctic has similarities to but also distinct differences from the stations further south. We note that this may change as the Arctic warms and sea ice continues to decline.
Bernadette Rosati, Sini Isokääntä, Sigurd Christiansen, Mads Mørk Jensen, Shamjad P. Moosakutty, Robin Wollesen de Jonge, Andreas Massling, Marianne Glasius, Jonas Elm, Annele Virtanen, and Merete Bilde
Atmos. Chem. Phys., 22, 13449–13466, https://doi.org/10.5194/acp-22-13449-2022, https://doi.org/10.5194/acp-22-13449-2022, 2022
Short summary
Short summary
Sulfate aerosols have a strong influence on climate. Due to the reduction in sulfur-based fossil fuels, natural sulfur emissions play an increasingly important role. Studies investigating the climate relevance of natural sulfur aerosols are scarce. We study the water uptake of such particles in the laboratory, demonstrating a high potential to take up water and form cloud droplets. During atmospheric transit, chemical processing affects the particles’ composition and thus their water uptake.
Jingwen Xue, Fangfang Ma, Jonas Elm, Jingwen Chen, and Hong-Bin Xie
Atmos. Chem. Phys., 22, 11543–11555, https://doi.org/10.5194/acp-22-11543-2022, https://doi.org/10.5194/acp-22-11543-2022, 2022
Short summary
Short summary
·OH/·Cl initiated indole reactions mainly form organonitrates, alkoxy radicals and hydroperoxide products, showing a varying mechanism from previously reported amines reactions. This study reveals carcinogenic nitrosamines cannot be formed in indole oxidation reactions despite radicals formed from -NH- H abstraction. The results are important to understand the atmospheric impact of indole oxidation and extend current understanding on the atmospheric chemistry of organic nitrogen compounds.
Ivo Beck, Hélène Angot, Andrea Baccarini, Lubna Dada, Lauriane Quéléver, Tuija Jokinen, Tiia Laurila, Markus Lampimäki, Nicolas Bukowiecki, Matthew Boyer, Xianda Gong, Martin Gysel-Beer, Tuukka Petäjä, Jian Wang, and Julia Schmale
Atmos. Meas. Tech., 15, 4195–4224, https://doi.org/10.5194/amt-15-4195-2022, https://doi.org/10.5194/amt-15-4195-2022, 2022
Short summary
Short summary
We present the pollution detection algorithm (PDA), a new method to identify local primary pollution in remote atmospheric aerosol and trace gas time series. The PDA identifies periods of contaminated data and relies only on the target dataset itself; i.e., it is independent of ancillary data such as meteorological variables. The parameters of all pollution identification steps are adjustable so that the PDA can be tuned to different locations and situations. It is available as open-access code.
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
Short summary
Short summary
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.
Lauriane L. J. Quéléver, Lubna Dada, Eija Asmi, Janne Lampilahti, Tommy Chan, Jonathan E. Ferrara, Gustavo E. Copes, German Pérez-Fogwill, Luis Barreira, Minna Aurela, Douglas R. Worsnop, Tuija Jokinen, and Mikko Sipilä
Atmos. Chem. Phys., 22, 8417–8437, https://doi.org/10.5194/acp-22-8417-2022, https://doi.org/10.5194/acp-22-8417-2022, 2022
Short summary
Short summary
Understanding how aerosols form is crucial for correctly modeling the climate and improving future predictions. This work provides extensive analysis of aerosol particles and their precursors at Marambio Station, Antarctic Peninsula. We show that sulfuric acid, ammonia, and dimethylamine are key contributors to the frequent new particle formation events observed at the site. We discuss nucleation mechanisms and highlight the need for targeted measurement to fully understand these processes.
Roseline C. Thakur, Lubna Dada, Lisa J. Beck, Lauriane L. J. Quéléver, Tommy Chan, Marjan Marbouti, Xu-Cheng He, Carlton Xavier, Juha Sulo, Janne Lampilahti, Markus Lampimäki, Yee Jun Tham, Nina Sarnela, Katrianne Lehtipalo, Alf Norkko, Markku Kulmala, Mikko Sipilä, and Tuija Jokinen
Atmos. Chem. Phys., 22, 6365–6391, https://doi.org/10.5194/acp-22-6365-2022, https://doi.org/10.5194/acp-22-6365-2022, 2022
Short summary
Short summary
Every year intense cyanobacterial and macroalgal blooms occur in the Baltic Sea and in the coastal areas surrounding Helsinki, yet no studies have addressed the impact of biogenic emissions from these blooms on gas vapor concentrations, which in turn could influence new particle formation. This is the first study of its kind to address the chemistry driving new particle formation (NPF) during a bloom period in this region, highlighting the role of biogenic sulfuric acid and iodic acid.
Yuanyuan Luo, Olga Garmash, Haiyan Li, Frans Graeffe, Arnaud P. Praplan, Anssi Liikanen, Yanjun Zhang, Melissa Meder, Otso Peräkylä, Josep Peñuelas, Ana María Yáñez-Serrano, and Mikael Ehn
Atmos. Chem. Phys., 22, 5619–5637, https://doi.org/10.5194/acp-22-5619-2022, https://doi.org/10.5194/acp-22-5619-2022, 2022
Short summary
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.
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
Short summary
Short summary
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.
Rongjie Zhang, Jiewen Shen, Hong-Bin Xie, Jingwen Chen, and Jonas Elm
Atmos. Chem. Phys., 22, 2639–2650, https://doi.org/10.5194/acp-22-2639-2022, https://doi.org/10.5194/acp-22-2639-2022, 2022
Short summary
Short summary
Formic acid is screened out as the species that can effectively catalyze the new particle formation (NPF) of the methanesulfonic acid (MSA)–methylamine system, indicating organic acids might be required to facilitate MSA-driven NPF in the atmosphere. The results are significant to comprehensively understand the MSA-driven NPF and expand current knowledge of the contribution of OAs to NPF.
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
Short summary
Short summary
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
Short summary
Short summary
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.
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
Short summary
Short summary
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.
Henrieka Detlef, Brendan Reilly, Anne Jennings, Mads Mørk Jensen, Matt O'Regan, Marianne Glasius, Jesper Olsen, Martin Jakobsson, and Christof Pearce
The Cryosphere, 15, 4357–4380, https://doi.org/10.5194/tc-15-4357-2021, https://doi.org/10.5194/tc-15-4357-2021, 2021
Short summary
Short summary
Here we examine the Nares Strait sea ice dynamics over the last 7000 years and their implications for the late Holocene readvance of the floating part of Petermann Glacier. We propose that the historically observed sea ice dynamics are a relatively recent feature, while most of the mid-Holocene was marked by variable sea ice conditions in Nares Strait. Nonetheless, major advances of the Petermann ice tongue were preceded by a shift towards harsher sea ice conditions in Nares Strait.
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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.
Robin Wollesen de Jonge, Jonas Elm, Bernadette Rosati, Sigurd Christiansen, Noora Hyttinen, Dana Lüdemann, Merete Bilde, and Pontus Roldin
Atmos. Chem. Phys., 21, 9955–9976, https://doi.org/10.5194/acp-21-9955-2021, https://doi.org/10.5194/acp-21-9955-2021, 2021
Short summary
Short summary
This study presents a detailed analysis of the OH-initiated oxidation of dimethyl sulfide (DMS) based on experiments performed in the Aarhus University Research on Aerosol (AURA) smog chamber and the gas- and particle-phase chemistry kinetic multilayer model (ADCHAM). We capture the formation, growth and chemical composition of aerosols in the chamber setup by an improved multiphase oxidation mechanism and utilize our results to reproduce the important role of DMS in the marine boundary layer.
Kai Wang, Ru-Jin Huang, Martin Brüggemann, Yun Zhang, Lu Yang, Haiyan Ni, Jie Guo, Meng Wang, Jiajun Han, Merete Bilde, Marianne Glasius, and Thorsten Hoffmann
Atmos. Chem. Phys., 21, 9089–9104, https://doi.org/10.5194/acp-21-9089-2021, https://doi.org/10.5194/acp-21-9089-2021, 2021
Short summary
Short summary
Here we present the detailed molecular composition of the organic aerosol collected in three eastern Chinese cities from north to south, Changchun, Shanghai and Guangzhou, by applying LC–Orbitrap analysis. Accordingly, the aromaticity degree of chemical compounds decreases from north to south, while the oxidation degree increases from north to south, which can be explained by the different anthropogenic emissions and photochemical oxidation processes.
Janne Lampilahti, Katri Leino, Antti Manninen, Pyry Poutanen, Anna Franck, Maija Peltola, Paula Hietala, Lisa Beck, Lubna Dada, Lauriane Quéléver, Ronja Öhrnberg, Ying Zhou, Madeleine Ekblom, Ville Vakkari, Sergej Zilitinkevich, Veli-Matti Kerminen, Tuukka Petäjä, and Markku Kulmala
Atmos. Chem. Phys., 21, 7901–7915, https://doi.org/10.5194/acp-21-7901-2021, https://doi.org/10.5194/acp-21-7901-2021, 2021
Short summary
Short summary
Using airborne measurements we observed increased number concentrations of sub-25 nm particles in the upper residual layer. These particles may be entrained into the well-mixed boundary layer and observed at the surface. We attribute our observations to new particle formation in the topmost part of the residual layer.
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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.
Noora Hyttinen, Reyhaneh Heshmatnezhad, Jonas Elm, Theo Kurtén, and Nønne L. Prisle
Atmos. Chem. Phys., 20, 13131–13143, https://doi.org/10.5194/acp-20-13131-2020, https://doi.org/10.5194/acp-20-13131-2020, 2020
Short summary
Short summary
We present aqueous solubilities and activity coefficients of mono- and dicarboxylic acids (C1–C6 and C2–C8, respectively) estimated using the COSMOtherm program. In addition, we have calculated effective equilibrium constants of dimerization and hydration of the same acids in the condensed phase. We were also able to improve the agreement between experimental and estimated properties of monocarboxylic acids in aqueous solutions by including clustering reactions in COSMOtherm calculations.
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
Short summary
Short summary
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.
Luisa Ickes, Grace C. E. Porter, Robert Wagner, Michael P. Adams, Sascha Bierbauer, Allan K. Bertram, Merete Bilde, Sigurd Christiansen, Annica M. L. Ekman, Elena Gorokhova, Kristina Höhler, Alexei A. Kiselev, Caroline Leck, Ottmar Möhler, Benjamin J. Murray, Thea Schiebel, Romy Ullrich, and Matthew E. Salter
Atmos. Chem. Phys., 20, 11089–11117, https://doi.org/10.5194/acp-20-11089-2020, https://doi.org/10.5194/acp-20-11089-2020, 2020
Short summary
Short summary
The Arctic is a region where aerosols are scarce. Sea spray might be a potential source of aerosols acting as ice-nucleating particles. We investigate two common phytoplankton species (Melosira arctica and Skeletonema marinoi) and present their ice nucleation activity in comparison with Arctic seawater microlayer samples from different field campaigns. We also aim to understand the aerosolization process of marine biological samples and the potential effect on the ice nucleation activity.
Cited articles
Atkinson, R., Winer, A. M., and Pitts, J. N.: Rate constants for the gas
phase reactions of O3 with the natural hydrocarbons isoprene and α-
and β-pinene, Atmos. Environ., 16, 1017–1020,
https://doi.org/10.1016/0004-6981(82)90187-1, 1982.
Beck, M. and Hoffmann, T.: A detailed MSn study for the molecular
identification of a dimer formed from oxidation of pinene, Atmos.
Environ., 130, 120–126, https://doi.org/10.1016/j.atmosenv.2015.09.012,
2016.
Berndt, T., Richters, S., Jokinen, T., Hyttinen, N., Kurtén, T.,
Otkjær, R. V., Kjaergaard, H. G., Stratmann, F., Herrmann, H., and
Sipilä, M.: Hydroxyl radical-induced formation of highly oxidized
organic compounds, Nat. Commun., 7, 13677, https://doi.org/10.1038/ncomms13677, 2016.
Berndt, T., Scholz, W., Mentler, B., Fischer, L., Herrmann, H., Kulmala, M.,
and Hansel, A.: Accretion Product Formation from Self- and Cross-Reactions
of RO2 Radicals in the Atmosphere, Angew. Chem. Int. Edit.,
57, 3820–3824, https://doi.org/10.1002/anie.201710989, 2018.
Bianchi, F., Kurtén, T., Riva, M., Mohr, C., Rissanen, M. P., Roldin,
P., Berndt, T., Crounse, J. D., Wennberg, P. O., Mentel, T. F., Wildt, J.,
Junninen, H., Jokinen, T., Kulmala, M., Worsnop, D. R., Thornton, J. A.,
Donahue, N., Kjaergaard, H. G., and Ehn, M.: Highly Oxygenated Organic
Molecules (HOM) from Gas-Phase Autoxidation Involving Peroxy Radicals: A Key
Contributor to Atmospheric Aerosol, Chem. Rev., 119, 3472–3509,
https://doi.org/10.1021/acs.chemrev.8b00395, 2019.
Bonn, B. and Moorgat, G. K.: New particle formation during a- and b-pinene oxidation by O3, OH and NO3, and the influence of water vapour: particle size distribution studies, Atmos. Chem. Phys., 2, 183–196, https://doi.org/10.5194/acp-2-183-2002, 2002.
Chhantyal-Pun, R., Rotavera, B., McGillen, M. R., Khan, M. A. H., Eskola, A.
J., Caravan, R. L., Blacker, L., Tew, D. P., Osborn, D. L., and Percival, C.
J.: Criegee intermediate reactions with carboxylic acids: a potential source
of secondary organic aerosol in the atmosphere, ACS Earth and Space
Chemistry, 2, 833–842, 2018.
Claeys, M., Iinuma, Y., Szmigielski, R., Surratt, J. D., Blockhuys, F., Van
Alsenoy, C., Boege, O., Sierau, B., Gomez-Gonzalez, Y., Vermeylen, R., Van
der Veken, P., Shahgholi, M., Chan, A. W. H., Herrmann, H., Seinfeld, J. H.,
and Maenhaut, W.: Terpenylic Acid and Related Compounds from the Oxidation
of alpha-Pinene: Implications for New Particle Formation and Growth above
Forests, Environ. Sci. Technol., 43, 6976–6982,
https://doi.org/10.1021/es9007596, 2009
Claflin, M. S., Krechmer, J. E., Hu, W., Jimenez, J. L., and Ziemann, P. J.:
Functional group composition of secondary organic aerosol formed from
ozonolysis of α-pinene under high VOC and autoxidation conditions,
ACS Earth and Space Chemistry, 2, 1196-1210, 2018.
Crounse, J. D., Nielsen, L. B., Jørgensen, S., Kjaergaard, H. G., and
Wennberg, P. O.: Autoxidation of Organic Compounds in the Atmosphere, The
J. Phys. Chem. Lett., 4, 3513–3520, https://doi.org/10.1021/jz4019207,
2013.
DeCarlo, P. F., Kimmel, J. R., Trimborn, A., Northway, M. J., Jayne, J. T.,
Aiken, A. C., Gonin, M., Fuhrer, K., Horvath, T., Docherty, K. S., Worsnop,
D. R., and Jimenez, J. L.: Field-Deployable, High-Resolution, Time-of-Flight
Aerosol Mass Spectrometer, Anal. Chem., 78, 8281–8289, https://doi.org/10.1021/ac061249n, 2006.
DePalma, J. W., Horan, A. J., Hall Iv, W. A., and Johnston, M. V.:
Thermodynamics of oligomer formation: implications for secondary organic
aerosol formation and reactivity, Phys. Chem. Chem. Phys., 15,
6935–6944, https://doi.org/10.1039/C3CP44586K, 2013.
Donahue, N. M., Henry, K. M., Mentel, T. F., Kiendler-Scharr, A., Spindler,
C., Bohn, B., Brauers, T., Dorn, H. P., Fuchs, H., and Tillmann, R.: Aging
of biogenic secondary organic aerosol via gas-phase OH radical reactions,
P. Natl. Acad. Sci. USA, 109, 13503–13508, 2012a.
Donahue, N. M., Kroll, J. H., Pandis, S. N., and Robinson, A. L.: A two-dimensional volatility basis set – Part 2: Diagnostics of organic-aerosol evolution, Atmos. Chem. Phys., 12, 615–634, https://doi.org/10.5194/acp-12-615-2012, 2012b.
Ehn, M., Thornton, J. A., Kleist, E., Sipilä, M., Junninen, H.,
Pullinen, I., Springer, M., Rubach, F., Tillmann, R., and Lee, B.: A large
source of low-volatility secondary organic aerosol, Nature, 506, 476–479, https://doi.org/10.1038/nature13032, 2014.
Ehn, M., Berndt, T., Wildt, J., and Mentel, T.: Highly Oxygenated Molecules
from Atmospheric Autoxidation of Hydrocarbons: A Prominent Challenge for
Chemical Kinetics Studies, Int. J. Chem. Kinet., 49, 821–831, https://doi.org/10.1002/kin.21130,
2017.
Elm, J.: Unexpected Growth Coordinate in Large Clusters Consisting of
Sulfuric Acid and C8H12O6 Tricarboxylic Acid, J. Phys.
Chem. A, 123, 3170–3175, https://doi.org/10.1021/acs.jpca.9b00428, 2019.
Elm, J., Myllys, N., and Kurtén, T.: What Is Required for Highly
Oxidized Molecules To Form Clusters with Sulfuric Acid?, J.
Phys. Chem. A, 121, 4578–4587, https://doi.org/10.1021/acs.jpca.7b03759, 2017.
Gao, S., Ng, N. L., Keywood, M., Varutbangkul, V., Bahreini, R., Nenes, A.,
He, J., Yoo, K. Y., Beauchamp, J., and Hodyss, R. P.: Particle phase acidity
and oligomer formation in secondary organic aerosol, Environ. Sci.
Technol., 38, 6582–6589, 2004.
Gao, Y., Hall, W. A., and Johnston, M. V.: Molecular Composition of
Monoterpene Secondary Organic Aerosol at Low Mass Loading, Environ.
Sci. Technol., 44, 7897–7902, https://doi.org/10.1021/es101861k, 2010.
Hakola, H., Tarvainen, V., Laurila, T., Hiltunen, V., Hellén, H., and
Keronen, P.: Seasonal variation of VOC concentrations above a boreal
coniferous forest, Atmos. Environ., 37, 1623–1634, 2003.
Hakola, H., Hellén, H., Tarvainen, V., Bäck, J., Patokoski, J., and
Rinne, J.: Annual variations of atmospheric VOC concentrations in a boreal
forest, Boreal Environ. Res., 14, 722–730, 2009.
Hoffmann, T., Bandur, R., Marggraf, U., and Linscheid, M.: Molecular
composition of organic aerosols formed in the α-pinene/O3 reaction:
Implications for new particle formation processes, J. Geophys.
Res.-Atmos., 103, 25569–25578, 1998
Huang, W., Saathoff, H., Pajunoja, A., Shen, X., Naumann, K.-H., Wagner, R., Virtanen, A., Leisner, T., and Mohr, C.: α-Pinene secondary organic aerosol at low temperature: chemical composition and implications for particle viscosity, Atmos. Chem. Phys., 18, 2883–2898, https://doi.org/10.5194/acp-18-2883-2018, 2018.
Jensen, L. N., Canagaratna, M. R., Kristensen, K., Quéléver, L. L. J., Rosati, B., Teiwes, R., Glasius, M., Pedersen, H. B., Ehn, M., and Bilde, M.: Temperature and VOC concentration as controlling factors for chemical composition of alpha-pinene derived secondary organic aerosol, Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-100, in review, 2020.
Jokinen, T., Sipilä, M., Junninen, H., Ehn, M., Lönn, G., Hakala, J., Petäjä, T., Mauldin III, R. L., Kulmala, M., and Worsnop, D. R.: Atmospheric sulphuric acid and neutral cluster measurements using CI-APi-TOF, Atmos. Chem. Phys., 12, 4117–4125, https://doi.org/10.5194/acp-12-4117-2012, 2012.
Jokinen, T., Sipilä, M., Richters, S., Kerminen, V.-M., Paasonen, P.,
Stratmann, F., Worsnop, D., Kulmala, M., Ehn, M., Herrmann, H., and Berndt,
T.: Rapid Autoxidation Forms Highly Oxidized RO2 Radicals in the Atmosphere,
Angew. Chem. Int. Edit., 53, 14596–14600, https://doi.org/10.1002/anie.201408566, 2014.
Jonsson, Å. M., Hallquist, M., and Ljungström, E.: The effect of temperature and water on secondary organic aerosol formation from ozonolysis of limonene, Δ3-carene and α-pinene, Atmos. Chem. Phys., 8, 6541–6549, https://doi.org/10.5194/acp-8-6541-2008, 2008.
Junninen, H., Ehn, M., Petäjä, T., Luosujärvi, L., Kotiaho, T., Kostiainen, R., Rohner, U., Gonin, M., Fuhrer, K., Kulmala, M., and Worsnop, D. R.: A high-resolution mass spectrometer to measure atmospheric ion composition, Atmos. Meas. Tech., 3, 1039–1053, https://doi.org/10.5194/amt-3-1039-2010, 2010.
Kahnt, A., Vermeylen, R., Iinuma, Y., Safi Shalamzari, M., Maenhaut, W., and Claeys, M.: High-molecular-weight esters in α-pinene ozonolysis secondary organic aerosol: structural characterization and mechanistic proposal for their formation from highly oxygenated molecules, Atmos. Chem. Phys., 18, 8453–8467, https://doi.org/10.5194/acp-18-8453-2018, 2018.
Kenseth, C. M., Huang, Y., Zhao, R., Dalleska, N. F., Hethcox, J. C.,
Stoltz, B. M., and Seinfeld, J. H.: Synergistic O3 + OH oxidation pathway
to extremely low-volatility dimers revealed in β-pinene secondary
organic aerosol, P. Natl. Acad. Sci. USA, 115,
8301–8306, https://doi.org/10.1073/pnas.1804671115, 2018.
Khan, M., Percival, C., Caravan, R., Taatjes, C., and Shallcross, D.:
Criegee intermediates and their impacts on the troposphere, Environ.
Sci.-Proc. Imp., 20, 437–453, 2018.
Kirkby, J., Duplissy, J., Sengupta, K., Frege, C., Gordon, H., Williamson,
C., Heinritzi, M., Simon, M., Yan, C., Almeida, J., Tröstl, J.,
Nieminen, T., Ortega, I. K., Wagner, R., Adamov, A., Amorim, A., Bernhammer,
A.-K., Bianchi, F., Breitenlechner, M., Brilke, S., Chen, X., Craven, J.,
Dias, A., Ehrhart, S., Flagan, R. C., Franchin, A., Fuchs, C., Guida, R.,
Hakala, J., Hoyle, C. R., Jokinen, T., Junninen, H., Kangasluoma, J., Kim,
J., Krapf, M., Kürten, A., Laaksonen, A., Lehtipalo, K., Makhmutov, V.,
Mathot, S., Molteni, U., Onnela, A., Peräkylä, O., Piel, F.,
Petäjä, T., Praplan, A. P., Pringle, K., Rap, A., Richards, N. A.
D., Riipinen, I., Rissanen, M. P., Rondo, L., Sarnela, N., Schobesberger,
S., Scott, C. E., Seinfeld, J. H., Sipilä, M., Steiner, G., Stozhkov,
Y., Stratmann, F., Tomé, A., Virtanen, A., Vogel, A. L., Wagner, A. C.,
Wagner, P. E., Weingartner, E., Wimmer, D., Winkler, P. M., Ye, P., Zhang,
X., Hansel, A., Dommen, J., Donahue, N. M., Worsnop, D. R., Baltensperger,
U., Kulmala, M., Carslaw, K. S., and Curtius, J.: Ion-induced nucleation of
pure biogenic particles, Nature, 533, 521–526, https://doi.org/10.1038/nature17953, 2016.
Kourtchev, I., Doussin, J.-F., Giorio, C., Mahon, B., Wilson, E. M., Maurin, N., Pangui, E., Venables, D. S., Wenger, J. C., and Kalberer, M.: Molecular composition of fresh and aged secondary organic aerosol from a mixture of biogenic volatile compounds: a high-resolution mass spectrometry study, Atmos. Chem. Phys., 15, 5683–5695, https://doi.org/10.5194/acp-15-5683-2015, 2015.
Kourtchev, I., Giorio, C., Manninen, A., Wilson, E., Mahon, B., Aalto, J.,
Kajos, M., Venables, D., Ruuskanen, T., and Levula, J.: Enhanced Volatile
Organic Compounds emissions and organic aerosol mass increase the oligomer
content of atmospheric aerosols, Sci. Rep., 6, 35038, https://doi.org/10.1038/srep35038, 2016.
Kristensen, K. and Glasius, M.: Organosulfates and oxidation products from
biogenic hydrocarbons in fine aerosols from a forest in North West Europe
during spring, Atmos. Environ., 45, 4546–4556, 2011.
Kristensen, K., Enggrob, K. L., King, S. M., Worton, D. R., Platt, S. M., Mortensen, R., Rosenoern, T., Surratt, J. D., Bilde, M., Goldstein, A. H., and Glasius, M.: Formation and occurrence of dimer esters of pinene oxidation products in atmospheric aerosols, Atmos. Chem. Phys., 13, 3763–3776, https://doi.org/10.5194/acp-13-3763-2013, 2013.
Kristensen, K., Cui, T., Zhang, H., Gold, A., Glasius, M., and Surratt, J. D.: Dimers in α-pinene secondary organic aerosol: effect of hydroxyl radical, ozone, relative humidity and aerosol acidity, Atmos. Chem. Phys., 14, 4201–4218, https://doi.org/10.5194/acp-14-4201-2014, 2014.
Kristensen, K., Watne, Å. K., Hammes, J., Lutz, A., Petäjä, T.,
Hallquist, M., Bilde, M., and Glasius, M.: High-Molecular Weight Dimer
Esters Are Major Products in Aerosols from α-Pinene Ozonolysis and
the Boreal Forest, Environ. Sci. Tech. Let., 3,
280–285, https://doi.org/10.1021/acs.estlett.6b00152, 2016.
Kristensen, K., Jensen, L., Glasius, M., and Bilde, M.: The effect of
sub-zero temperature on the formation and composition of secondary organic
aerosol from ozonolysis of alpha-pinene, Enviro. Sci.-Proc.
Imp., 19, 1220–1234, 2017.
Kroll, J. H. and Seinfeld, J. H.: Chemistry of secondary organic aerosol:
Formation and evolution of low-volatility organics in the atmosphere,
Atmos. Environ., 42, 3593–3624, 2008.
Kulmala, M., Kontkanen, J., Junninen, H., Lehtipalo, K., Manninen, H. E.,
Nieminen, T., Petäjä, T., Sipilä, M., Schobesberger, S., and
Rantala, P.: Direct observations of atmospheric aerosol nucleation, Science,
339, 943–946, 2013.
Kurteìn, T., Tiusanen, K., Roldin, P., Rissanen, M., Luy, J.-N., Boy, M.,
Ehn, M., and Donahue, N.: α-Pinene autoxidation products may not
have extremely low saturation vapor pressures despite high O:C ratios,
J. Phys. Chem. A, 120, 2569–2582, 2016.
Lawler, M. J., Rissanen, M. P., Ehn, M., Mauldin III, R. L., Sarnela, N.,
Sipilä, M., and Smith, J. N.: Evidence for diverse biogeochemical
drivers of boreal forest new particle formation, Geophys. Res.
Lett., 45, 2038–2046, 2018.
Lee, B. H., D'Ambro, E. L., Lopez-Hilfiker, F. D., Schobesberger, S., Mohr,
C., Zawadowicz, M. A., Liu, J., Shilling, J. E., Hu, W., Palm, B. B.,
Jimenez, J. L., Hao, L., Virtanen, A., Zhang, H., Goldstein, A. H., Pye, H.
O. T., and Thornton, J. A.: Resolving Ambient Organic Aerosol Formation and
Aging Pathways with Simultaneous Molecular Composition and Volatility
Observations, ACS Earth and Space Chemistry, 4, 391–402, https://doi.org/10.1021/acsearthspacechem.9b00302, 2020.
Lee, S. and Kamens, R. M.: Particle nucleation from the reaction of α-pinene and O3, Atmos. Environ., 39, 6822–6832,
https://doi.org/10.1016/j.atmosenv.2005.07.062, 2005.
Lee, S. H., Uin, J., Guenther, A. B., de Gouw, J. A., Yu, F., Nadykto, A.
B., Herb, J., Ng, N. L., Koss, A., and Brune, W. H.: Isoprene suppression of
new particle formation: Potential mechanisms and implications, J.
Geophys. Res.-Atmos., 121, 14621–14635, 2016.
Li, Y. and Shiraiwa, M.: Timescales of secondary organic aerosols to reach equilibrium at various temperatures and relative humidities, Atmos. Chem. Phys., 19, 5959–5971, https://doi.org/10.5194/acp-19-5959-2019, 2019.
McGillen, M. R., Curchod, B. F., Chhantyal-Pun, R., Beames, J. M., Watson,
N., Khan, M. A. H., McMahon, L., Shallcross, D. E., and Orr-Ewing, A. J.:
Criegee intermediate–alcohol reactions, a potential source of
functionalized hydroperoxides in the atmosphere, ACS Earth and Space
Chemistry, 1, 664–672, 2017.
Metzger, A., Verheggen, B., Dommen, J., Duplissy, J., Prevot, A. S.,
Weingartner, E., Riipinen, I., Kulmala, M., Spracklen, D. V., and Carslaw,
K. S.: Evidence for the role of organics in aerosol particle formation under
atmospheric conditions, P. Natl. Acad. Sci. USA,
107, 6646–6651, 2010.
Mohr, C., Lopez-Hilfiker, F. D., Yli-Juuti, T., Heitto, A., Lutz, A.,
Hallquist, M., D'Ambro, E. L., Rissanen, M. P., Hao, L., and Schobesberger,
S.: Ambient observations of dimers from terpene oxidation in the gas phase:
Implications for new particle formation and growth, Geophys. Res.
Lett., 44, 2958–2966, 2017.
Müller, L., Reinnig, M.-C., Naumann, K. H., Saathoff, H., Mentel, T. F., Donahue, N. M., and Hoffmann, T.: Formation of 3-methyl-1,2,3-butanetricarboxylic acid via gas phase oxidation of pinonic acid – a mass spectrometric study of SOA aging, Atmos. Chem. Phys., 12, 1483–1496, https://doi.org/10.5194/acp-12-1483-2012, 2012.
Mutzel, A., Poulain, L., Berndt, T., Iinuma, Y., Rodigast, M., Böge, O.,
Richters, S., Spindler, G., Sipilä, M., Jokinen, T., Kulmala, M., and
Herrmann, H.: Highly Oxidized Multifunctional Organic Compounds Observed in
Tropospheric Particles: A Field and Laboratory Study, Environ. Sci.
Technol., 49, 7754–7761, https://doi.org/10.1021/acs.est.5b00885, 2015.
Nizkorodov, S. A., Laskin, J., and Laskin, A.: Molecular chemistry of
organic aerosols through the application of high resolution mass
spectrometry, Phys. Chem. Chem. Phys., 13, 3612–3629, 2011.
Noe, S. M., Hüve, K., Niinemets, Ü., and Copolovici, L.: Seasonal variation in vertical volatile compounds air concentrations within a remote hemiboreal mixed forest, Atmos. Chem. Phys., 12, 3909–3926, https://doi.org/10.5194/acp-12-3909-2012, 2012.
Noziere, B., Kalberer, M., Claeys, M., Allan, J., D'Anna, B., Decesari, S.,
Finessi, E., Glasius, M., Grgic, I., and Hamilton, J. F.: The molecular
identification of organic compounds in the atmosphere: state of the art and
challenges, Chem. Rev., 115, 3919-3983, 2015.
Pathak, R. K., Stanier, C. O., Donahue, N. M., and Pandis, S. N.: Ozonolysis
of α-pinene at atmospherically relevant concentrations: Temperature
dependence of aerosol mass fractions (yields), J. Geophys.
Res.-Atmos., 112, D03201, https://doi.org/10.1029/2006JD007436, 2007.
Peräkylä, O., Riva, M., Heikkinen, L., Quéléver, L., Roldin, P., and Ehn, M.: Experimental investigation into the volatilities of highly oxygenated organic molecules (HOMs) , Atmos. Chem. Phys., 20, 649–669, https://doi.org/10.5194/acp-20-649-2020, 2020.
Quéléver, L. L. J., Kristensen, K., Normann Jensen, L., Rosati, B., Teiwes, R., Daellenbach, K. R., Peräkylä, O., Roldin, P., Bossi, R., Pedersen, H. B., Glasius, M., Bilde, M., and Ehn, M.: Effect of temperature on the formation of highly oxygenated organic molecules (HOMs) from alpha-pinene ozonolysis, Atmos. Chem. Phys., 19, 7609–7625, https://doi.org/10.5194/acp-19-7609-2019, 2019.
Renbaum-Wolff, L., Grayson, J. W., Bateman, A. P., Kuwata, M., Sellier, M.,
Murray, B. J., Shilling, J. E., Martin, S. T., and Bertram, A. K.: Viscosity
of α-pinene
secondary organic material and implications for particle growth and
reactivity, P. Natl. Acad. Sci. USA, 110, 8014–8019, https://doi.org/10.1073/pnas.1219548110, 2013.
Riccobono, F., Schobesberger, S., Scott, C. E., Dommen, J., Ortega, I. K.,
Rondo, L., Almeida, J., Amorim, A., Bianchi, F., and Breitenlechner, M.:
Oxidation products of biogenic emissions contribute to nucleation of
atmospheric particles, Science, 344, 717–721, 2014.
Rissanen, M. P., Kurtén, T., Sipilä, M., Thornton, J. A., Kausiala,
O., Garmash, O., Kjaergaard, H. G., Petäjä, T., Worsnop, D. R., Ehn,
M., and Kulmala, M.: Effects of Chemical Complexity on the Autoxidation
Mechanisms of Endocyclic Alkene Ozonolysis Products: From Methylcyclohexenes
toward Understanding α-Pinene, J. Phys. Chem. A,
119, 4633–4650, https://doi.org/10.1021/jp510966g, 2015.
Rosati, B., Teiwes, R., Kristensen, K., Bossi, R., Skov, H., Glasius, M.,
Pedersen, H. B., and Bilde, M.: Factor analysis of chemical ionization
experiments: Numerical simulations and an experimental case study of the
ozonolysis of α-pinene using a PTR-ToF-MS, Atmos. Environ.,
199, 15–31, https://doi.org/10.1016/j.atmosenv.2018.11.012, 2019.
Saathoff, H., Naumann, K.-H., Möhler, O., Jonsson, Å. M., Hallquist, M., Kiendler-Scharr, A., Mentel, Th. F., Tillmann, R., and Schurath, U.: Temperature dependence of yields of secondary organic aerosols from the ozonolysis of α-pinene and limonene, Atmos. Chem. Phys., 9, 1551–1577, https://doi.org/10.5194/acp-9-1551-2009, 2009.
Shiraiwa, M. and Seinfeld, J. H.: Equilibration timescale of atmospheric
secondary organic aerosol partitioning, Geophys. Res. Lett., 39, L24801, https://doi.org/10.1029/2012GL054008,
2012.
Simon, M., Dada, L., Heinritzi, M., Scholz, W., Stolzenburg, D., Fischer, L., Wagner, A. C., Kürten, A., Rörup, B., He, X.-C., Almeida, J., Baalbaki, R., Baccarini, A., Bauer, P. S., Beck, L., Bergen, A., Bianchi, F., Bräkling, S., Brilke, S., Caudillo, L., Chen, D., Chu, B., Dias, A., Draper, D. C., Duplissy, J., El-Haddad, I., Finkenzeller, H., Frege, C., Gonzalez-Carracedo, L., Gordon, H., Granzin, M., Hakala, J., Hofbauer, V., Hoyle, C. R., Kim, C., Kong, W., Lamkaddam, H., Lee, C. P., Lehtipalo, K., Leiminger, M., Mai, H., Manninen, H. E., Marie, G., Marten, R., Mentler, B., Molteni, U., Nichman, L., Nie, W., Ojdanic, A., Onnela, A., Partoll, E., Petäjä, T., Pfeifer, J., Philippov, M., Quéléver, L. L. J., Ranjithkumar, A., Rissanen, M. P., Schallhart, S., Schobesberger, S., Schuchmann, S., Shen, J., Sipilä, M., Steiner, G., Stozhkov, Y., Tauber, C., Tham, Y. J., Tomé, A. R., Vazquez-Pufleau, M., Vogel, A. L., Wagner, R., Wang, M., Wang, D. S., Wang, Y., Weber, S. K., Wu, Y., Xiao, M., Yan, C., Ye, P., Ye, Q., Zauner-Wieczorek, M., Zhou, X., Baltensperger, U., Dommen, J., Flagan, R. C., Hansel, A., Kulmala, M., Volkamer, R., Winkler, P. M., Worsnop, D. R., Donahue, N. M., Kirkby, J., and Curtius, J.: Molecular understanding of new-particle formation from α-pinene between −50 and +25 ∘C, Atmos. Chem. Phys., 20, 9183–9207, https://doi.org/10.5194/acp-20-9183-2020, 2020.
Sindelarova, K., Granier, C., Bouarar, I., Guenther, A., Tilmes, S., Stavrakou, T., Müller, J.-F., Kuhn, U., Stefani, P., and Knorr, W.: Global data set of biogenic VOC emissions calculated by the MEGAN model over the last 30 years, Atmos. Chem. Phys., 14, 9317–9341, https://doi.org/10.5194/acp-14-9317-2014, 2014.
Stolzenburg, D., Fischer, L., Vogel, A. L., Heinritzi, M., Schervish, M.,
Simon, M., Wagner, A. C., Dada, L., Ahonen, L. R., Amorim, A., Baccarini,
A., Bauer, P. S., Baumgartner, B., Bergen, A., Bianchi, F., Breitenlechner,
M., Brilke, S., Buenrostro Mazon, S., Chen, D., Dias, A., Draper, D. C.,
Duplissy, J., El Haddad, I., Finkenzeller, H., Frege, C., Fuchs, C.,
Garmash, O., Gordon, H., He, X., Helm, J., Hofbauer, V., Hoyle, C. R., Kim,
C., Kirkby, J., Kontkanen, J., Kürten, A., Lampilahti, J., Lawler, M.,
Lehtipalo, K., Leiminger, M., Mai, H., Mathot, S., Mentler, B., Molteni, U.,
Nie, W., Nieminen, T., Nowak, J. B., Ojdanic, A., Onnela, A., Passananti,
M., Petäjä, T., Quéléver, L. L. J., Rissanen, M. P.,
Sarnela, N., Schallhart, S., Tauber, C., Tomé, A., Wagner, R., Wang, M.,
Weitz, L., Wimmer, D., Xiao, M., Yan, C., Ye, P., Zha, Q., Baltensperger,
U., Curtius, J., Dommen, J., Flagan, R. C., Kulmala, M., Smith, J. N.,
Worsnop, D. R., Hansel, A., Donahue, N. M., and Winkler, P. M.: Rapid growth
of organic aerosol nanoparticles over a wide tropospheric temperature range,
P. Natl. Acad. Sci. USA, 115, 9122–9127, https://doi.org/10.1073/pnas.1807604115, 2018.
Svendby, T. M., Lazaridis, M., and Tørseth, K.: Temperature dependent
secondary organic aerosol formation from terpenes and aromatics, J.
Atmos. Chem., 59, 25–46, https://doi.org/10.1007/s10874-007-9093-7, 2008.
Szmigielski, R., Surratt, J. D., Gómez-González, Y., Van der Veken,
P., Kourtchev, I., Vermeylen, R., Blockhuys, F., Jaoui, M., Kleindienst, T.
E., and Lewandowski, M.: 3-methyl-1, 2, 3-butanetricarboxylic acid: An
atmospheric tracer for terpene secondary organic aerosol, Geophys.
Res. Lett., 34, L24811, https://doi.org/10.1029/2007GL031338, 2007.
Tillmann, R., Hallquist, M., Jonsson, Å. M., Kiendler-Scharr, A., Saathoff, H., Iinuma, Y., and Mentel, Th. F.: Influence of relative humidity and temperature on the production of pinonaldehyde and OH radicals from the ozonolysis of α-pinene, Atmos. Chem. Phys., 10, 7057–7072, https://doi.org/10.5194/acp-10-7057-2010, 2010.
Tolocka, M. P., Jang, M., Ginter, J. M., Cox, F. J., Kamens, R. M., and
Johnston, M. V.: Formation of Oligomers in Secondary Organic Aerosol,
Environ. Sci. Technol., 38, 1428–1434, https://doi.org/10.1021/es035030r,
2004.
Tolocka, M. P., Heaton, K. J., Dreyfus, M. A., Wang, S., Zordan, C. A.,
Saul, T. D., and Johnston, M. V.: Chemistry of Particle Inception and Growth
during α-Pinene Ozonolysis, Environ. Sci. Technol.,
40, 1843–1848, https://doi.org/10.1021/es051926f, 2006.
Tröstl, J., Chuang, W. K., Gordon, H., Heinritzi, M., Yan, C., Molteni,
U., Ahlm, L., Frege, C., Bianchi, F., and Wagner, R.: The role of
low-volatility organic compounds in initial particle growth in the
atmosphere, Nature, 533, 527–531, https://doi.org/10.1038/nature18271
2016.
Vanhanen, J., Mikkilä, J., Lehtipalo, K., Sipilä, M., Manninen, H.
E., Siivola, E., Petäjä, T., and Kulmala, M.: Particle Size
Magnifier for Nano-CN Detection, Aerosol Sci. Tech., 45,
533–542, https://doi.org/10.1080/02786826.2010.547889, 2011.
Vereecken, L., Müller, J.-F., and Peeters, J.: Low-volatility
poly-oxygenates in the OH-initiated atmospheric oxidation of α-pinene: impact of non-traditional peroxyl radical chemistry, Phys.
Chem. Chem. Phys., 9, 5241–5248, 2007.
von Hessberg, C., von Hessberg, P., Pöschl, U., Bilde, M., Nielsen, O. J., and Moortgat, G. K.: Temperature and humidity dependence of secondary organic aerosol yield from the ozonolysis of β-pinene, Atmos. Chem. Phys., 9, 3583–3599, https://doi.org/10.5194/acp-9-3583-2009, 2009.
Warren, B., Austin, R. L., and Cocker, D. R.: Temperature dependence of
secondary organic aerosol, Atmos. Environ., 43, 3548–3555, https://doi.org/10.1016/j.atmosenv.2009.04.011, 2009.
Witkowski, B. and Gierczak, T.: Early stage composition of SOA produced by
α-pinene/ozone reaction: α-Acyloxyhydroperoxy aldehydes and
acidic dimers, Atmos. Environ., 95, 59–70, 2014.
Yasmeen, F., Vermeylen, R., Szmigielski, R., Iinuma, Y., Böge, O., Herrmann, H., Maenhaut, W., and Claeys, M.: Terpenylic acid and related compounds: precursors for dimers in secondary organic aerosol from the ozonolysis of α- and β-pinene, Atmos. Chem. Phys., 10, 9383–9392, https://doi.org/10.5194/acp-10-9383-2010, 2010.
Zaveri, R. A., Easter, R. C., Shilling, J. E., and Seinfeld, J. H.: Modeling kinetic partitioning of secondary organic aerosol and size distribution dynamics: representing effects of volatility, phase state, and particle-phase reaction, Atmos. Chem. Phys., 14, 5153–5181, https://doi.org/10.5194/acp-14-5153-2014, 2014.
Zaveri, R. A., Shilling, J. E., Zelenyuk, A., Zawadowicz, M. A., Suski, K.,
China, S., Bell, D. M., Veghte, D., and Laskin, A.: Particle-Phase Diffusion
Modulates Partitioning of Semivolatile Organic Compounds to Aged Secondary
Organic Aerosol, Environ. Sci. Technol., 54, 2595–2605, https://doi.org/10.1021/acs.est.9b05514, 2020.
Zhang, H., Yee, L. D., Lee, B. H., Curtis, M. P., Worton, D. R.,
Isaacman-VanWertz, G., Offenberg, J. H., Lewandowski, M., Kleindienst, T.
E., and Beaver, M. R.: Monoterpenes are the largest source of summertime
organic aerosol in the southeastern United States, P.
Natl. Acad. Sci. USA, 115, 2038–2043, 2018.
Zhang, X., McVay, R. C., Huang, D. D., Dalleska, N. F., Aumont, B., Flagan,
R. C., and Seinfeld, J. H.: Formation and evolution of molecular products in
α-pinene secondary organic aerosol, P. Natl.
Acad. Sci. USA, 112, 14168–14173, 2015.
Zhang, X., Lambe, A. T., Upshur, M. A., Brooks, W. A., Gray Beì, A.,
Thomson, R. J., Geiger, F. M., Surratt, J. D., Zhang, Z., and Gold, A.:
Highly oxygenated multifunctional compounds in α-pinene secondary
organic aerosol, Environ. Sci. Technol., 51, 5932–5940, 2017.
Zhao, R., Kenseth, C. M., Huang, Y., Dalleska, N. F., Kuang, X. M., Chen,
J., Paulson, S. E., and Seinfeld, J. H.: Rapid Aqueous-Phase Hydrolysis of
Ester Hydroperoxides Arising from Criegee Intermediates and Organic Acids,
J. Phys. Chem. A, 122, 5190–5201, 2018a.
Zhao, Y., Wingen, L. M., Perraud, V., Greaves, J., and Finlayson-Pitts, B.
J.: Role of the reaction of stabilized Criegee intermediates with peroxy
radicals in particle formation and growth in air, Phys. Chem.
Chem. Phys., 17, 12500–12514, 2015.
Zhao, Y., Thornton, J. A., and Pye, H. O.: Quantitative constraints on
autoxidation and dimer formation from direct probing of monoterpene-derived
peroxy radical chemistry, P. Natl. Acad. Sci. USA,
115, 12142–12147, 2018b.
Zhao, Z., Le, C., Xu, Q., Peng, W., Jiang, H., Lin, Y.-H., Cocker, D. R.,
and Zhang, H.: Compositional Evolution of Secondary Organic Aerosol as
Temperature and Relative Humidity Cycle in Atmospherically Relevant Ranges,
ACS Earth and Space Chemistry, 3, 2549–2558, https://doi.org/10.1021/acsearthspacechem.9b00232, 2019a.
Zhao, Z., Tolentino, R., Lee, J., Vuong, A., Yang, X., and Zhang, H.:
Interfacial dimerization by organic radical reactions during heterogeneous
oxidative aging of oxygenated organic aerosols, J. Phys.
Chem. A, 123, 10782–10792, 2019b.
Short summary
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.
Atmospheric particles are important in relation to human health and the global climate. As the...
Altmetrics
Final-revised paper
Preprint