Articles | Volume 18, issue 23
https://doi.org/10.5194/acp-18-17589-2018
© Author(s) 2018. 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-18-17589-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
12 Dec 2018
Research article |
| 12 Dec 2018
| 12 Dec 2018
Estimating the saturation vapor pressures of isoprene oxidation products C5H12O6 and C5H10O6 using COSMO-RS
Theo Kurtén
CORRESPONDING AUTHOR
University of Helsinki, Department of Chemistry and Institute for
Atmospheric and Earth System Research (INAR), P.O. Box 55, 00014 Helsinki, Finland
Noora Hyttinen
University of Helsinki, Department of Chemistry and Institute for
Atmospheric and Earth System Research (INAR), P.O. Box 55, 00014 Helsinki, Finland
Emma Louise D'Ambro
Department of Chemistry, University of Washington, Seattle, Washington
98195, USA
Department of Atmospheric Sciences, University of Washington, Seattle,
Washington 98195, USA
Joel Thornton
Department of Chemistry, University of Washington, Seattle, Washington
98195, USA
Department of Atmospheric Sciences, University of Washington, Seattle,
Washington 98195, USA
Nønne Lyng Prisle
University of Oulu, Nano and Molecular Systems Research Unit, P.O. Box
3000, 90014 Oulu, Finland
Related authors
Alfred W. Mayhew, Lauri Franzon, Kelvin H. Bates, Theo Kurtén, Felipe D. Lopez-Hilfiker, Claudia Mohr, Andrew R. Rickard, Joel A. Thornton, and Jessica D. Haskins
EGUsphere, https://doi.org/10.5194/egusphere-2025-1922, https://doi.org/10.5194/egusphere-2025-1922, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
Short summary
Short summary
This work outlines an investigation into an understudied atmospheric chemical reaction pathway with the potential to form particulate pollution that has important impacts on air quality and climate. We suggest that this chemical pathway is responsible for a large fraction of the atmospheric particulate matter observed in tropical forested regions, but we also highlight the need for further ambient and lab investigations to inform an accurate representation of this process in atmospheric models.
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.
Lauri Franzon, Marie Camredon, Richard Valorso, Bernard Aumont, and Theo Kurtén
Atmos. Chem. Phys., 24, 11679–11699, https://doi.org/10.5194/acp-24-11679-2024, https://doi.org/10.5194/acp-24-11679-2024, 2024
Short summary
Short summary
In this article we investigate the formation of large, sticky molecules from various organic compounds entering the atmosphere as primary emissions and the degree to which these processes may contribute to organic aerosol particle mass. More specifically, we qualitatively investigate a recently discovered chemical reaction channel for one of the most important short-lived radical compounds, peroxy radicals, and discover which of these reactions are most atmospherically important.
Lukas Pichelstorfer, Pontus Roldin, Matti Rissanen, Noora Hyttinen, Olga Garmash, Carlton Xavier, Putian Zhou, Petri Clusius, Benjamin Foreback, Thomas Golin Almeida, Chenjuan Deng, Metin Baykara, Theo Kurten, and Michael Boy
EGUsphere, https://doi.org/10.5194/egusphere-2023-1415, https://doi.org/10.5194/egusphere-2023-1415, 2023
Preprint archived
Short summary
Short summary
Secondary organic aerosols (SOA) form effectively from gaseous precursors via a process called autoxidation. While key chemical reaction types seem to be known, no general description of autoxidation chemistry exists. In the present work, we present a method to create autoxidation chemistry schemes for any atmospherically relevant hydrocarbon. We exemplarily investigate benzene and its potential to form aerosols. We found that autoxidation, under some conditions, can dominate the SOA formation.
Huan Yang, Ivo Neefjes, Valtteri Tikkanen, Jakub Kubečka, Theo Kurtén, Hanna Vehkamäki, and Bernhard Reischl
Atmos. Chem. Phys., 23, 5993–6009, https://doi.org/10.5194/acp-23-5993-2023, https://doi.org/10.5194/acp-23-5993-2023, 2023
Short summary
Short summary
We present a new analytical model for collision rates between molecules and clusters of arbitrary sizes, accounting for long-range interactions. The model is verified against atomistic simulations of typical acid–base clusters participating in atmospheric new particle formation (NPF). Compared to non-interacting models, accounting for long-range interactions leads to 2–3 times higher collision rates for small clusters, indicating the necessity of including such interactions in NPF modeling.
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.
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.
Emma Lumiaro, Milica Todorović, Theo Kurten, Hanna Vehkamäki, and Patrick Rinke
Atmos. Chem. Phys., 21, 13227–13246, https://doi.org/10.5194/acp-21-13227-2021, https://doi.org/10.5194/acp-21-13227-2021, 2021
Short summary
Short summary
The study of climate change relies on climate models, which require an understanding of aerosol formation. We train a machine-learning model to predict the partitioning coefficients of atmospheric molecules, which govern condensation into aerosols. The model can make instant predictions based on molecular structures with accuracy surpassing that of standard computational methods. This will allow the screening of low-volatility molecules that contribute most to aerosol formation.
Xiaolong Fan, Jing Cai, Chao Yan, Jian Zhao, Yishuo Guo, Chang Li, Kaspar R. Dällenbach, Feixue Zheng, Zhuohui Lin, Biwu Chu, Yonghong Wang, Lubna Dada, Qiaozhi Zha, Wei Du, Jenni Kontkanen, Theo Kurtén, Siddhart Iyer, Joni T. Kujansuu, Tuukka Petäjä, Douglas R. Worsnop, Veli-Matti Kerminen, Yongchun Liu, Federico Bianchi, Yee Jun Tham, Lei Yao, and Markku Kulmala
Atmos. Chem. Phys., 21, 11437–11452, https://doi.org/10.5194/acp-21-11437-2021, https://doi.org/10.5194/acp-21-11437-2021, 2021
Short summary
Short summary
We observed significant concentrations of gaseous HBr and HCl throughout the winter and springtime in urban Beijing, China. Our results indicate that gaseous HCl and HBr are most likely originated from anthropogenic emissions such as burning activities, and the gas–aerosol partitioning may play a crucial role in contributing to the gaseous HCl and HBr. These observations suggest that there is an important recycling pathway of halogen species in inland megacities.
Mingyi Wang, Xu-Cheng He, Henning Finkenzeller, Siddharth Iyer, Dexian Chen, Jiali Shen, Mario Simon, Victoria Hofbauer, Jasper Kirkby, Joachim Curtius, Norbert Maier, Theo Kurtén, Douglas R. Worsnop, Markku Kulmala, Matti Rissanen, Rainer Volkamer, Yee Jun Tham, Neil M. Donahue, and Mikko Sipilä
Atmos. Meas. Tech., 14, 4187–4202, https://doi.org/10.5194/amt-14-4187-2021, https://doi.org/10.5194/amt-14-4187-2021, 2021
Short summary
Short summary
Atmospheric iodine species are often short-lived with low abundance and have thus been challenging to measure. We show that the bromide chemical ionization mass spectrometry, compatible with both the atmospheric pressure and reduced pressure interfaces, can simultaneously detect various gas-phase iodine species. Combining calibration experiments and quantum chemical calculations, we quantify detection sensitivities to HOI, HIO3, I2, and H2SO4, giving detection limits down to < 106 molec. cm-3.
Georgia Michailoudi, Jack J. Lin, Hayato Yuzawa, Masanari Nagasaka, Marko Huttula, Nobuhiro Kosugi, Theo Kurtén, Minna Patanen, and Nønne L. Prisle
Atmos. Chem. Phys., 21, 2881–2894, https://doi.org/10.5194/acp-21-2881-2021, https://doi.org/10.5194/acp-21-2881-2021, 2021
Short summary
Short summary
This study provides insight into hydration of two significant atmospheric compounds, glyoxal and methylglyoxal. Using synchrotron radiation excited X-ray absorption spectroscopy, we confirm that glyoxal is fully hydrated in water, and for the first time, we experimentally detect enol structures in aqueous methylglyoxal. Our results support the contribution of these compounds to secondary organic aerosol formation, known to have a large uncertainty in atmospheric models and climate predictions.
Anna Shcherbacheva, Tracey Balehowsky, Jakub Kubečka, Tinja Olenius, Tapio Helin, Heikki Haario, Marko Laine, Theo Kurtén, and Hanna Vehkamäki
Atmos. Chem. Phys., 20, 15867–15906, https://doi.org/10.5194/acp-20-15867-2020, https://doi.org/10.5194/acp-20-15867-2020, 2020
Short summary
Short summary
Atmospheric new particle formation and cluster growth to aerosol particles is an important field of research, in particular due to the climate change phenomenon. Evaporation rates are very difficult to account for but they are important to explain the formation and growth of particles. Different quantum chemistry (QC) methods produce substantially different values for the evaporation rates. We propose a novel approach for inferring evaporation rates of clusters from available measurements.
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.
Tommaso Zanca, Jakub Kubečka, Evgeni Zapadinsky, Monica Passananti, Theo Kurtén, and Hanna Vehkamäki
Atmos. Meas. Tech., 13, 3581–3593, https://doi.org/10.5194/amt-13-3581-2020, https://doi.org/10.5194/amt-13-3581-2020, 2020
Short summary
Short summary
In this paper we quantify (using a statistical model) the probability of decomposition of a representative class of HOM clusters in an APi-TOF mass spectrometer. This is important because it quantifies the systematic error of measurements in a APi-TOF MS due to cluster decomposition. The results (specific for our selected clusters) show that decomposition is negligible, provided their bonding energy is large enough to allow formation in the atmosphere in the first place.
Roope Halonen, Evgeni Zapadinsky, Theo Kurtén, Hanna Vehkamäki, and Bernhard Reischl
Atmos. Chem. Phys., 19, 13355–13366, https://doi.org/10.5194/acp-19-13355-2019, https://doi.org/10.5194/acp-19-13355-2019, 2019
Short summary
Short summary
The rate of collisions between molecules or clusters is used to determine particle formation in the atmosphere. The basic approach is to treat the colliding particles as noninteracting hard spheres. By using atomistic simulations with a realistic force field and theoretical approaches, we showed that the actual collision rate of two sulfuric acid molecules is more than twice as high as that for hard spheres. The results of this study will improve models of atmospheric particle growth.
Emma L. D'Ambro, Siegfried Schobesberger, Cassandra J. Gaston, Felipe D. Lopez-Hilfiker, Ben H. Lee, Jiumeng Liu, Alla Zelenyuk, David Bell, Christopher D. Cappa, Taylor Helgestad, Ziyue Li, Alex Guenther, Jian Wang, Matthew Wise, Ryan Caylor, Jason D. Surratt, Theran Riedel, Noora Hyttinen, Vili-Taneli Salo, Galib Hasan, Theo Kurtén, John E. Shilling, and Joel A. Thornton
Atmos. Chem. Phys., 19, 11253–11265, https://doi.org/10.5194/acp-19-11253-2019, https://doi.org/10.5194/acp-19-11253-2019, 2019
Short summary
Short summary
Isoprene is the most abundantly emitted reactive organic gas globally, and thus it is important to understand its fate and role in aerosol formation and growth. A major product of its oxidation is an epoxydiol, IEPOX, which can be efficiently taken up by acidic aerosol to generate substantial amounts of secondary organic aerosol (SOA). We present chamber experiments exploring the properties of IEPOX SOA and reconcile discrepancies between field, laboratory, and model studies of this process.
Ulrich K. Krieger, Franziska Siegrist, Claudia Marcolli, Eva U. Emanuelsson, Freya M. Gøbel, Merete Bilde, Aleksandra Marsh, Jonathan P. Reid, Andrew J. Huisman, Ilona Riipinen, Noora Hyttinen, Nanna Myllys, Theo Kurtén, Thomas Bannan, Carl J. Percival, and David Topping
Atmos. Meas. Tech., 11, 49–63, https://doi.org/10.5194/amt-11-49-2018, https://doi.org/10.5194/amt-11-49-2018, 2018
Short summary
Short summary
Vapor pressures of low-volatility organic molecules at atmospheric temperatures reported in the literature often differ by several orders of magnitude between measurement techniques. These discrepancies exceed the stated uncertainty of each technique, which is generally reported to be smaller than a factor of 2. We determined saturation vapor pressures for the homologous series of polyethylene glycols ranging in vapor pressure at 298 K from 1E−7 Pa to 5E−2 Pa as a reference set.
Emilie Öström, Zhou Putian, Guy Schurgers, Mikhail Mishurov, Niku Kivekäs, Heikki Lihavainen, Mikael Ehn, Matti P. Rissanen, Theo Kurtén, Michael Boy, Erik Swietlicki, and Pontus Roldin
Atmos. Chem. Phys., 17, 8887–8901, https://doi.org/10.5194/acp-17-8887-2017, https://doi.org/10.5194/acp-17-8887-2017, 2017
Short summary
Short summary
We used a model to study how biogenic volatile organic compounds (BVOCs) emitted from the boreal forest contribute to the formation and growth of particles in the atmosphere. Some of these particles are important climate forcers, acting as seeds for cloud droplet fomation. We implemented a new gas chemistry mechanism that describes how the BVOCs are oxidized and form low-volatility highly oxidized organic molecules. With the new mechanism we are able to accurately predict the particle growth.
Hanna K. Lappalainen, Veli-Matti Kerminen, Tuukka Petäjä, Theo Kurten, Aleksander Baklanov, Anatoly Shvidenko, Jaana Bäck, Timo Vihma, Pavel Alekseychik, Meinrat O. Andreae, Stephen R. Arnold, Mikhail Arshinov, Eija Asmi, Boris Belan, Leonid Bobylev, Sergey Chalov, Yafang Cheng, Natalia Chubarova, Gerrit de Leeuw, Aijun Ding, Sergey Dobrolyubov, Sergei Dubtsov, Egor Dyukarev, Nikolai Elansky, Kostas Eleftheriadis, Igor Esau, Nikolay Filatov, Mikhail Flint, Congbin Fu, Olga Glezer, Aleksander Gliko, Martin Heimann, Albert A. M. Holtslag, Urmas Hõrrak, Juha Janhunen, Sirkku Juhola, Leena Järvi, Heikki Järvinen, Anna Kanukhina, Pavel Konstantinov, Vladimir Kotlyakov, Antti-Jussi Kieloaho, Alexander S. Komarov, Joni Kujansuu, Ilmo Kukkonen, Ella-Maria Duplissy, Ari Laaksonen, Tuomas Laurila, Heikki Lihavainen, Alexander Lisitzin, Alexsander Mahura, Alexander Makshtas, Evgeny Mareev, Stephany Mazon, Dmitry Matishov, Vladimir Melnikov, Eugene Mikhailov, Dmitri Moisseev, Robert Nigmatulin, Steffen M. Noe, Anne Ojala, Mari Pihlatie, Olga Popovicheva, Jukka Pumpanen, Tatjana Regerand, Irina Repina, Aleksei Shcherbinin, Vladimir Shevchenko, Mikko Sipilä, Andrey Skorokhod, Dominick V. Spracklen, Hang Su, Dmitry A. Subetto, Junying Sun, Arkady Y. Terzhevik, Yuri Timofeyev, Yuliya Troitskaya, Veli-Pekka Tynkkynen, Viacheslav I. Kharuk, Nina Zaytseva, Jiahua Zhang, Yrjö Viisanen, Timo Vesala, Pertti Hari, Hans Christen Hansson, Gennady G. Matvienko, Nikolai S. Kasimov, Huadong Guo, Valery Bondur, Sergej Zilitinkevich, and Markku Kulmala
Atmos. Chem. Phys., 16, 14421–14461, https://doi.org/10.5194/acp-16-14421-2016, https://doi.org/10.5194/acp-16-14421-2016, 2016
Short summary
Short summary
After kick off in 2012, the Pan-Eurasian Experiment (PEEX) program has expanded fast and today the multi-disciplinary research community covers ca. 80 institutes and a network of ca. 500 scientists from Europe, Russia, and China. Here we introduce scientific topics relevant in this context. This is one of the first multi-disciplinary overviews crossing scientific boundaries, from atmospheric sciences to socio-economics and social sciences.
Felipe D. Lopez-Hilfiker, Siddarth Iyer, Claudia Mohr, Ben H. Lee, Emma L. D'Ambro, Theo Kurtén, and Joel A. Thornton
Atmos. Meas. Tech., 9, 1505–1512, https://doi.org/10.5194/amt-9-1505-2016, https://doi.org/10.5194/amt-9-1505-2016, 2016
Short summary
Short summary
We present the maximum sensitivity of a TOF-CIMS using the collision limit and iodide adducts. We also present an ion adduct declustering scanning procedure which determines the effective binding energies of the detected ion adducts and therefore their approximate sensitivity. The combination of declustering scanning and the collision limit provides an approximate calibration for many compounds in the mass spectrum which would otherwise be impossible to obtain by traditional methods.
M. Kulmala, H. K. Lappalainen, T. Petäjä, T. Kurten, V.-M. Kerminen, Y. Viisanen, P. Hari, S. Sorvari, J. Bäck, V. Bondur, N. Kasimov, V. Kotlyakov, G. Matvienko, A. Baklanov, H. D. Guo, A. Ding, H.-C. Hansson, and S. Zilitinkevich
Atmos. Chem. Phys., 15, 13085–13096, https://doi.org/10.5194/acp-15-13085-2015, https://doi.org/10.5194/acp-15-13085-2015, 2015
Short summary
Short summary
The Pan-European Experiment (PEEX) is introduced. PEEX is a multidisciplinary, multiscale and multicomponent research, research infrastructure and capacity-building program. This paper outlines the mission, vision and objectives of PEEX and introduces its main components, including the research agenda, research infrastructure, knowledge transfer and potential impacts on society. The paper also summarizes the main scientific questions that PEEX is going to tackle in the future.
K. Ruusuvuori, P. Hietala, O. Kupiainen-Määttä, T. Jokinen, H. Junninen, M. Sipilä, T. Kurtén, and H. Vehkamäki
Atmos. Meas. Tech., 8, 2577–2588, https://doi.org/10.5194/amt-8-2577-2015, https://doi.org/10.5194/amt-8-2577-2015, 2015
Short summary
Short summary
Ionization reagents suitable for accurate measurements of the atmospheric gas-phase amine vapour concentrations are needed. Based on computational results, acetone is a viable option for use as an ionization reagent in CI-APi-TOF measurements on atmospheric dimethylamine. However, comparison between the computational and experimental results revealed notable discrepancies. Further study is still required before the acetone CI-APi-TOF can be considered a viable option in practice.
T. F. Mentel, M. Springer, M. Ehn, E. Kleist, I. Pullinen, T. Kurtén, M. Rissanen, A. Wahner, and J. Wildt
Atmos. Chem. Phys., 15, 6745–6765, https://doi.org/10.5194/acp-15-6745-2015, https://doi.org/10.5194/acp-15-6745-2015, 2015
Short summary
Short summary
We studied a series of cycloalkenes and methyl-substituted alkenes in order to elucidate the structural pre-requisites and chemical pathways to the recently discovered class of highly oxidized molecules ELVOC (Ehn et al., Nature, 2014). ELVOC may totally change the view on (parts of) the mechanism of SOA formation. We present results which support recent observations of H shifts from C-H to peroxy radicals, highlighting the pivotal role of peroxyradicals in organic atmospheric chemistry.
M. Sipilä, T. Jokinen, T. Berndt, S. Richters, R. Makkonen, N. M. Donahue, R. L. Mauldin III, T. Kurtén, P. Paasonen, N. Sarnela, M. Ehn, H. Junninen, M. P. Rissanen, J. Thornton, F. Stratmann, H. Herrmann, D. R. Worsnop, M. Kulmala, V.-M. Kerminen, and T. Petäjä
Atmos. Chem. Phys., 14, 12143–12153, https://doi.org/10.5194/acp-14-12143-2014, https://doi.org/10.5194/acp-14-12143-2014, 2014
I. K. Ortega, T. Olenius, O. Kupiainen-Määttä, V. Loukonen, T. Kurtén, and H. Vehkamäki
Atmos. Chem. Phys., 14, 7995–8007, https://doi.org/10.5194/acp-14-7995-2014, https://doi.org/10.5194/acp-14-7995-2014, 2014
K. Ruusuvuori, T. Kurtén, I. K. Ortega, J. Faust, and H. Vehkamäki
Atmos. Chem. Phys., 13, 10397–10404, https://doi.org/10.5194/acp-13-10397-2013, https://doi.org/10.5194/acp-13-10397-2013, 2013
N. Bork, T. Kurtén, and H. Vehkamäki
Atmos. Chem. Phys., 13, 3695–3703, https://doi.org/10.5194/acp-13-3695-2013, https://doi.org/10.5194/acp-13-3695-2013, 2013
Alison Bain, Kunal Ghosh, Konstantin Tumashevich, Nønne L. Prisle, and Bryan R. Bzdek
Atmos. Chem. Phys., 25, 5633–5645, https://doi.org/10.5194/acp-25-5633-2025, https://doi.org/10.5194/acp-25-5633-2025, 2025
Short summary
Short summary
We measure the surface tension of picoliter-volume droplets containing strong ionic surfactants and cosolutes and compare this to surface tension predictions using two independent surfactant partitioning models. Under high-water-activity conditions, experimental measurements and model predictions show no change when NaCl cosolute is replaced with sea salt. Model predictions show that total surfactant concentrations in the range of tens to hundreds of millimolar are required to lower the surface tension of accumulation-mode aerosol.
Arttu Ylisirniö, Noora Hyttinen, Zijun Li, Mitchell Alton, Aki Nissinen, Iida Pullinen, Pasi Miettinen, Taina Yli-Juuti, and Siegfried Schobesberger
EGUsphere, https://doi.org/10.5194/egusphere-2025-2219, https://doi.org/10.5194/egusphere-2025-2219, 2025
This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
Short summary
Short summary
This study aims to increase knowledge of the low volatility organic compouds observed in ambient aerosol particles by providing new volatility information about compounds used for calibrating volatility measurement instruments. Previously, such information has was not available and calibration of the instrument had to be extrapolated to cover the whole measurement range. Results of this study will provide the scientific community better tools for investigating the complexity of ambient aerosols.
Joseph O. Palmo, Colette L. Heald, Donald R. Blake, Ilann Bourgeois, Matthew Coggon, Jeff Collett, Frank Flocke, Alan Fried, Georgios Gkatzelis, Samuel Hall, Lu Hu, Jose L. Jimenez, Pedro Campuzano-Jost, I-Ting Ku, Benjamin Nault, Brett Palm, Jeff Peischl, Ilana Pollack, Amy Sullivan, Joel Thornton, Carsten Warneke, Armin Wisthaler, and Lu Xu
EGUsphere, https://doi.org/10.5194/egusphere-2025-1969, https://doi.org/10.5194/egusphere-2025-1969, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
Short summary
Short summary
This study investigates ozone production within wildfire smoke plumes as they age, using both aircraft observations and models. We find that the chemical environment and resulting ozone production within smoke changes as plumes evolve, with implications for climate and public health.
Xinyue Shao, Yaman Liu, Xinyi Dong, Minghuai Wang, Ruochong Xu, Joel A. Thornton, Duseong S. Jo, Man Yue, Wenxiang Shen, Manish Shrivastava, Stephen R. Arnold, and Ken S. Carslaw
EGUsphere, https://doi.org/10.5194/egusphere-2025-1526, https://doi.org/10.5194/egusphere-2025-1526, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
Short summary
Short summary
Highly Oxygenated Organic Molecules (HOMs) are key precursors of secondary organic aerosols (SOA). Incorporating the HOMs chemical mechanism into a global climate model allows for a reasonable reproduction of observed HOM characteristics. HOM-SOA constitutes a significant fraction of global SOA, and its distribution and formation pathways exhibit strong sensitivity to uncertainties in autoxidation processes and peroxy radical branching ratios.
Alfred W. Mayhew, Lauri Franzon, Kelvin H. Bates, Theo Kurtén, Felipe D. Lopez-Hilfiker, Claudia Mohr, Andrew R. Rickard, Joel A. Thornton, and Jessica D. Haskins
EGUsphere, https://doi.org/10.5194/egusphere-2025-1922, https://doi.org/10.5194/egusphere-2025-1922, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
Short summary
Short summary
This work outlines an investigation into an understudied atmospheric chemical reaction pathway with the potential to form particulate pollution that has important impacts on air quality and climate. We suggest that this chemical pathway is responsible for a large fraction of the atmospheric particulate matter observed in tropical forested regions, but we also highlight the need for further ambient and lab investigations to inform an accurate representation of this process in atmospheric models.
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.
Chris J. Wright, Joel A. Thornton, Lyatt Jaeglé, Yang Cao, Yannian Zhu, Jihu Liu, Randall Jones II, Robert Holzworth, Daniel Rosenfeld, Robert Wood, Peter Blossey, and Daehyun Kim
Atmos. Chem. Phys., 25, 2937–2946, https://doi.org/10.5194/acp-25-2937-2025, https://doi.org/10.5194/acp-25-2937-2025, 2025
Short summary
Short summary
Aerosol particles influence clouds, which exert a large forcing on solar radiation and freshwater. To better understand the mechanisms by which aerosol influences thunderstorms, we look at the two busiest shipping lanes in the world, where recent regulations have reduced sulfur emissions by nearly an order of magnitude. We find that the reduction in emissions has been accompanied by a dramatic decrease in both lightning and the number of droplets in clouds over the shipping lanes.
Delaney B. Kilgour, Christopher M. Jernigan, Olga Garmash, Sneha Aggarwal, Shengqian Zhou, Claudia Mohr, Matt E. Salter, Joel A. Thornton, Jian Wang, Paul Zieger, and Timothy H. Bertram
Atmos. Chem. Phys., 25, 1931–1947, https://doi.org/10.5194/acp-25-1931-2025, https://doi.org/10.5194/acp-25-1931-2025, 2025
Short summary
Short summary
We report simultaneous measurements of dimethyl sulfide (DMS) and hydroperoxymethyl thioformate (HPMTF) in the eastern North Atlantic. We use an observationally constrained box model to show that cloud loss is the dominant sink of HPMTF in this region over 6 weeks, resulting in large reductions in DMS-derived products that contribute to aerosol formation and growth. Our findings indicate that fast cloud processing of HPMTF must be included in global models to accurately capture the sulfur cycle.
T. Nash Skipper, Emma L. D'Ambro, Forwood C. Wiser, V. Faye McNeill, Rebecca H. Schwantes, Barron H. Henderson, Ivan R. Piletic, Colleen B. Baublitz, Jesse O. Bash, Andrew R. Whitehill, Lukas C. Valin, Asher P. Mouat, Jennifer Kaiser, Glenn M. Wolfe, Jason M. St. Clair, Thomas F. Hanisco, Alan Fried, Bryan K. Place, and Havala O.T. Pye
Atmos. Chem. Phys., 24, 12903–12924, https://doi.org/10.5194/acp-24-12903-2024, https://doi.org/10.5194/acp-24-12903-2024, 2024
Short summary
Short summary
We develop the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM) version 2 to improve predictions of formaldehyde in ambient air compared to satellite-, aircraft-, and ground-based observations. With the updated chemistry, we estimate the cancer risk from inhalation exposure to ambient formaldehyde across the contiguous USA and predict that 40 % of this risk is controllable through reductions in anthropogenic emissions of nitrogen oxides and reactive organic carbon.
Lauri Franzon, Marie Camredon, Richard Valorso, Bernard Aumont, and Theo Kurtén
Atmos. Chem. Phys., 24, 11679–11699, https://doi.org/10.5194/acp-24-11679-2024, https://doi.org/10.5194/acp-24-11679-2024, 2024
Short summary
Short summary
In this article we investigate the formation of large, sticky molecules from various organic compounds entering the atmosphere as primary emissions and the degree to which these processes may contribute to organic aerosol particle mass. More specifically, we qualitatively investigate a recently discovered chemical reaction channel for one of the most important short-lived radical compounds, peroxy radicals, and discover which of these reactions are most atmospherically important.
Zijun Li, Angela Buchholz, and Noora Hyttinen
Atmos. Chem. Phys., 24, 11717–11725, https://doi.org/10.5194/acp-24-11717-2024, https://doi.org/10.5194/acp-24-11717-2024, 2024
Short summary
Short summary
Evaluating organosulfur (OS) hygroscopicity is important for assessing aerosol–cloud climate interactions in the post-fossil-fuel future, when SO2 emissions decrease and OS compounds become increasingly important. Here a state-of-the-art quantum-chemistry-based method was used to predict the hygroscopic growth factors (HGFs) of a group of atmospherically relevant OS compounds and their mixtures with (NH4)2SO4. A good agreement was observed between their model-estimated and experimental HGFs.
Matthieu Riva, Veronika Pospisilova, Carla Frege, Sebastien Perrier, Priyanka Bansal, Spiro Jorga, Patrick Sturm, Joel A. Thornton, Urs Rohner, and Felipe Lopez-Hilfiker
Atmos. Meas. Tech., 17, 5887–5901, https://doi.org/10.5194/amt-17-5887-2024, https://doi.org/10.5194/amt-17-5887-2024, 2024
Short summary
Short summary
We present a newly designed reduced-pressure chemical ionization reactor for detection of gas-phase organic and inorganic species. The system operates through the combined use of vacuum ultraviolet ionization and photosensitizers to generate numerous adduct ionization schemes. As a result, it offers the ability to simultaneously measure a wide variety of organic and inorganic species in terms of compound volatility and functionality, while being largely independent of changes in sample humidity.
Carley D. Fredrickson, Scott J. Janz, Lok N. Lamsal, Ursula A. Jongebloed, Joshua L. Laughner, and Joel A. Thornton
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2024-158, https://doi.org/10.5194/amt-2024-158, 2024
Revised manuscript accepted for AMT
Short summary
Short summary
We present an analysis of high-resolution remote sensing measurements of nitrogen-containing trace gases emitted by wildfires. The measurements were made using an instrument on the NASA ER-2 aircraft in the summer of 2019. We find that time-resolved fire intensity is critical to quantify trace gas emissions over a fire’s entire lifespan. These findings have implications for improving air pollution forecasts downwind of wildfires using computer models of atmospheric chemistry and meteorology.
Chuanyang Shen, Xiaoyan Yang, Joel Thornton, John Shilling, Chenyang Bi, Gabriel Isaacman-VanWertz, and Haofei Zhang
Atmos. Chem. Phys., 24, 6153–6175, https://doi.org/10.5194/acp-24-6153-2024, https://doi.org/10.5194/acp-24-6153-2024, 2024
Short summary
Short summary
In this work, a condensed multiphase isoprene oxidation mechanism was developed to simulate isoprene SOA formation from chamber and field studies. Our results show that the measured isoprene SOA mass concentrations can be reasonably reproduced. The simulation results indicate that multifunctional low-volatility products contribute significantly to total isoprene SOA. Our findings emphasize that the pathways to produce these low-volatility species should be considered in models.
Wei Huang, Cheng Wu, Linyu Gao, Yvette Gramlich, Sophie L. Haslett, Joel Thornton, Felipe D. Lopez-Hilfiker, Ben H. Lee, Junwei Song, Harald Saathoff, Xiaoli Shen, Ramakrishna Ramisetty, Sachchida N. Tripathi, Dilip Ganguly, Feng Jiang, Magdalena Vallon, Siegfried Schobesberger, Taina Yli-Juuti, and Claudia Mohr
Atmos. Chem. Phys., 24, 2607–2624, https://doi.org/10.5194/acp-24-2607-2024, https://doi.org/10.5194/acp-24-2607-2024, 2024
Short summary
Short summary
We present distinct molecular composition and volatility of oxygenated organic aerosol particles in different rural, urban, and mountain environments. We do a comprehensive investigation of the relationship between the chemical composition and volatility of oxygenated organic aerosol particles across different systems and environments. This study provides implications for volatility descriptions of oxygenated organic aerosol particles in different model frameworks.
Gargi Sengupta, Minjie Zheng, and Nønne L. Prisle
Atmos. Chem. Phys., 24, 1467–1487, https://doi.org/10.5194/acp-24-1467-2024, https://doi.org/10.5194/acp-24-1467-2024, 2024
Short summary
Short summary
The effect of organic acid aerosol on sulfur chemistry and cloud properties was investigated in an atmospheric model. Organic acid dissociation was considered using both bulk and surface-related properties. We found that organic acid dissociation leads to increased hydrogen ion concentrations and sulfate aerosol mass in aqueous aerosols, increasing cloud formation. This could be important in large-scale climate models as many organic aerosol components are both acidic and surface-active.
Sampo Vepsäläinen, Silvia M. Calderón, and Nønne L. Prisle
Atmos. Chem. Phys., 23, 15149–15164, https://doi.org/10.5194/acp-23-15149-2023, https://doi.org/10.5194/acp-23-15149-2023, 2023
Short summary
Short summary
Atmospheric aerosols act as seeds for cloud formation. Many aerosols contain surface active material that accumulates at the surface of growing droplets. This can affect cloud droplet activation, but the broad significance of the effect and the best way to model it are still debated. We compare predictions of six models to surface activity of strongly surface active aerosol and find significant differences between the models, especially with large fractions of surfactant in the dry particles.
Minjie Zheng, Hongyu Liu, Florian Adolphi, Raimund Muscheler, Zhengyao Lu, Mousong Wu, and Nønne L. Prisle
Geosci. Model Dev., 16, 7037–7057, https://doi.org/10.5194/gmd-16-7037-2023, https://doi.org/10.5194/gmd-16-7037-2023, 2023
Short summary
Short summary
The radionuclides 7Be and 10Be are useful tracers for atmospheric transport studies. Here we use the GEOS-Chem to simulate 7Be and 10Be with different production rates: the default production rate in GEOS-Chem and two from the state-of-the-art beryllium production model. We demonstrate that reduced uncertainties in the production rates can enhance the utility of 7Be and 10Be as tracers for evaluating transport and scavenging processes in global models.
Noora Hyttinen
Atmos. Chem. Phys., 23, 13809–13817, https://doi.org/10.5194/acp-23-13809-2023, https://doi.org/10.5194/acp-23-13809-2023, 2023
Short summary
Short summary
Water activity in aerosol particles describes how particles respond to variations in relative humidity. Here, water activities were calculated for a set of 80 salts that may be present in aerosol particles using a state-of-the-art quantum-chemistry-based method. The effect of the dissociated salt on water activity varies with both the cation and anion. Most of the studied salts increase water uptake compared to pure water-soluble organic particles.
Bryan K. Place, William T. Hutzell, K. Wyat Appel, Sara Farrell, Lukas Valin, Benjamin N. Murphy, Karl M. Seltzer, Golam Sarwar, Christine Allen, Ivan R. Piletic, Emma L. D'Ambro, Emily Saunders, Heather Simon, Ana Torres-Vasquez, Jonathan Pleim, Rebecca H. Schwantes, Matthew M. Coggon, Lu Xu, William R. Stockwell, and Havala O. T. Pye
Atmos. Chem. Phys., 23, 9173–9190, https://doi.org/10.5194/acp-23-9173-2023, https://doi.org/10.5194/acp-23-9173-2023, 2023
Short summary
Short summary
Ground-level ozone is a pollutant with adverse human health and ecosystem effects. Air quality models allow scientists to understand the chemical production of ozone and demonstrate impacts of air quality management plans. In this work, the role of multiple systems in ozone production was investigated for the northeastern US in summer. Model updates to chemical reaction rates and monoterpene chemistry were most influential in decreasing predicted ozone and improving agreement with observations.
Sophie L. Haslett, David M. Bell, Varun Kumar, Jay G. Slowik, Dongyu S. Wang, Suneeti Mishra, Neeraj Rastogi, Atinderpal Singh, Dilip Ganguly, Joel Thornton, Feixue Zheng, Yuanyuan Li, Wei Nie, Yongchun Liu, Wei Ma, Chao Yan, Markku Kulmala, Kaspar R. Daellenbach, David Hadden, Urs Baltensperger, Andre S. H. Prevot, Sachchida N. Tripathi, and Claudia Mohr
Atmos. Chem. Phys., 23, 9023–9036, https://doi.org/10.5194/acp-23-9023-2023, https://doi.org/10.5194/acp-23-9023-2023, 2023
Short summary
Short summary
In Delhi, some aspects of daytime and nighttime atmospheric chemistry are inverted, and parodoxically, vehicle emissions may be limiting other forms of particle production. This is because the nighttime emissions of nitrogen oxide (NO) by traffic and biomass burning prevent some chemical processes that would otherwise create even more particles and worsen the urban haze.
Lukas Pichelstorfer, Pontus Roldin, Matti Rissanen, Noora Hyttinen, Olga Garmash, Carlton Xavier, Putian Zhou, Petri Clusius, Benjamin Foreback, Thomas Golin Almeida, Chenjuan Deng, Metin Baykara, Theo Kurten, and Michael Boy
EGUsphere, https://doi.org/10.5194/egusphere-2023-1415, https://doi.org/10.5194/egusphere-2023-1415, 2023
Preprint archived
Short summary
Short summary
Secondary organic aerosols (SOA) form effectively from gaseous precursors via a process called autoxidation. While key chemical reaction types seem to be known, no general description of autoxidation chemistry exists. In the present work, we present a method to create autoxidation chemistry schemes for any atmospherically relevant hydrocarbon. We exemplarily investigate benzene and its potential to form aerosols. We found that autoxidation, under some conditions, can dominate the SOA formation.
Zijun Li, Noora Hyttinen, Miika Vainikka, Olli-Pekka Tikkasalo, Siegfried Schobesberger, and Taina Yli-Juuti
Atmos. Chem. Phys., 23, 6863–6877, https://doi.org/10.5194/acp-23-6863-2023, https://doi.org/10.5194/acp-23-6863-2023, 2023
Short summary
Short summary
The saturation vapor pressure (psat) of low-volatility organic compounds (LVOCs) governs their partitioning between the gas and particle phases. To estimate the psat of selected LVOCs, we performed particle evaporation measurements in a residence time chamber at a temperature setting relevant to atmospheric aerosol formation and conducted state-of-the-art computational calculations. We found good agreement between the experimentally measured and model-estimated psat values for most LVOCs.
Huan Yang, Ivo Neefjes, Valtteri Tikkanen, Jakub Kubečka, Theo Kurtén, Hanna Vehkamäki, and Bernhard Reischl
Atmos. Chem. Phys., 23, 5993–6009, https://doi.org/10.5194/acp-23-5993-2023, https://doi.org/10.5194/acp-23-5993-2023, 2023
Short summary
Short summary
We present a new analytical model for collision rates between molecules and clusters of arbitrary sizes, accounting for long-range interactions. The model is verified against atomistic simulations of typical acid–base clusters participating in atmospheric new particle formation (NPF). Compared to non-interacting models, accounting for long-range interactions leads to 2–3 times higher collision rates for small clusters, indicating the necessity of including such interactions in NPF modeling.
Havala O. T. Pye, Bryan K. Place, Benjamin N. Murphy, Karl M. Seltzer, Emma L. D'Ambro, Christine Allen, Ivan R. Piletic, Sara Farrell, Rebecca H. Schwantes, Matthew M. Coggon, Emily Saunders, Lu Xu, Golam Sarwar, William T. Hutzell, Kristen M. Foley, George Pouliot, Jesse Bash, and William R. Stockwell
Atmos. Chem. Phys., 23, 5043–5099, https://doi.org/10.5194/acp-23-5043-2023, https://doi.org/10.5194/acp-23-5043-2023, 2023
Short summary
Short summary
Chemical mechanisms describe how emissions from vehicles, vegetation, and other sources are chemically transformed in the atmosphere to secondary products including criteria and hazardous air pollutants. The Community Regional Atmospheric Chemistry Multiphase Mechanism integrates gas-phase radical chemistry with pathways to fine-particle mass. New species were implemented, resulting in a bottom-up representation of organic aerosol, which is required for accurate source attribution of pollutants.
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.
Siegfried Schobesberger, Emma L. D'Ambro, Lejish Vettikkat, Ben H. Lee, Qiaoyun Peng, David M. Bell, John E. Shilling, Manish Shrivastava, Mikhail Pekour, Jerome Fast, and Joel A. Thornton
Atmos. Meas. Tech., 16, 247–271, https://doi.org/10.5194/amt-16-247-2023, https://doi.org/10.5194/amt-16-247-2023, 2023
Short summary
Short summary
We present a new, highly sensitive technique for measuring atmospheric ammonia, an important trace gas that is emitted mainly by agriculture. We deployed the instrument on an aircraft during research flights over rural Oklahoma. Due to its fast response, we could analyze correlations with turbulent winds and calculate ammonia emissions from nearby areas at 1 to 2 km resolution. We observed high spatial variability and point sources that are not resolved in the US National Emissions Inventory.
Alfred W. Mayhew, Ben H. Lee, Joel A. Thornton, Thomas J. Bannan, James Brean, James R. Hopkins, James D. Lee, Beth S. Nelson, Carl Percival, Andrew R. Rickard, Marvin D. Shaw, Peter M. Edwards, and Jaqueline F. Hamilton
Atmos. Chem. Phys., 22, 14783–14798, https://doi.org/10.5194/acp-22-14783-2022, https://doi.org/10.5194/acp-22-14783-2022, 2022
Short summary
Short summary
Isoprene nitrates are chemical species commonly found in the atmosphere that are important for their impacts on air quality and climate. This paper compares 3 different representations of the chemistry of isoprene nitrates in computational models highlighting cases where the choice of chemistry included has significant impacts on the concentration and composition of the modelled nitrates. Calibration of mass spectrometers is also shown to be an important factor when analysing isoprene nitrates.
Ruochong Xu, Joel A. Thornton, Ben H. Lee, Yanxu Zhang, Lyatt Jaeglé, Felipe D. Lopez-Hilfiker, Pekka Rantala, and Tuukka Petäjä
Atmos. Chem. Phys., 22, 5477–5494, https://doi.org/10.5194/acp-22-5477-2022, https://doi.org/10.5194/acp-22-5477-2022, 2022
Short summary
Short summary
Monoterpenes are emitted into the atmosphere by vegetation and by the use of certain consumer products. Reactions of monoterpenes in the atmosphere lead to low-volatility products that condense to grow particulate matter or participate in new particle formation and, thus, affect air quality and climate. We use a model of atmospheric chemistry and transport to evaluate the global-scale importance of recent updates to our understanding of monoterpene chemistry in particle formation and growth.
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.
Sampo Vepsäläinen, Silvia M. Calderón, Jussi Malila, and Nønne L. Prisle
Atmos. Chem. Phys., 22, 2669–2687, https://doi.org/10.5194/acp-22-2669-2022, https://doi.org/10.5194/acp-22-2669-2022, 2022
Short summary
Short summary
Atmospheric aerosols act as seeds for cloud formation. Many aerosols contain surface active material that accumulates at the surface of growing droplets. This can affect cloud droplet activation, but the broad significance of the effect and the best way to model it are still debated. We compare predictions of six different model approaches to surface activity of organic aerosols and find significant differences between the models, especially with large fractions of organics in the dry particles.
Noora Hyttinen, Iida Pullinen, Aki Nissinen, Siegfried Schobesberger, Annele Virtanen, and Taina Yli-Juuti
Atmos. Chem. Phys., 22, 1195–1208, https://doi.org/10.5194/acp-22-1195-2022, https://doi.org/10.5194/acp-22-1195-2022, 2022
Short summary
Short summary
Accurate saturation vapor pressure estimates of atmospherically relevant organic compounds are critical for modeling secondary organic aerosol (SOA) formation. We investigated vapor pressures of highly oxygenated SOA constituents using state-of-the-art computational and experimental methods. We found a good agreement between low and extremely low vapor pressures estimated using the two methods, and the smallest molecules detected in our experiment were likely products of thermal decomposition.
Arto Heitto, Kari Lehtinen, Tuukka Petäjä, Felipe Lopez-Hilfiker, Joel A. Thornton, Markku Kulmala, and Taina Yli-Juuti
Atmos. Chem. Phys., 22, 155–171, https://doi.org/10.5194/acp-22-155-2022, https://doi.org/10.5194/acp-22-155-2022, 2022
Short summary
Short summary
For atmospheric aerosol particles to take part in cloud formation, they need to be at least a few tens of nanometers in diameter. By using a particle condensation model, we investigated how two types of chemical reactions, oligomerization and decomposition, of organic molecules inside the particle may affect the growth of secondary aerosol particles to these sizes. We show that the effect is potentially significant, which highlights the importance of increasing understanding of these processes.
Nønne L. Prisle
Atmos. Chem. Phys., 21, 16387–16411, https://doi.org/10.5194/acp-21-16387-2021, https://doi.org/10.5194/acp-21-16387-2021, 2021
Short summary
Short summary
A mass-based Gibbs adsorption model is presented to enable predictive Köhler calculations of droplet growth and activation with considerations of surface partitioning, surface tension, and non-ideal water activity for chemically complex and unresolved surface active aerosol mixtures, including actual atmospheric samples. The model is used to calculate cloud condensation nuclei (CCN) activity of aerosol particles comprising strongly surface-active model atmospheric humic-like substances (HULIS).
Zachary C. J. Decker, Michael A. Robinson, Kelley C. Barsanti, Ilann Bourgeois, Matthew M. Coggon, Joshua P. DiGangi, Glenn S. Diskin, Frank M. Flocke, Alessandro Franchin, Carley D. Fredrickson, Georgios I. Gkatzelis, Samuel R. Hall, Hannah Halliday, Christopher D. Holmes, L. Gregory Huey, Young Ro Lee, Jakob Lindaas, Ann M. Middlebrook, Denise D. Montzka, Richard Moore, J. Andrew Neuman, John B. Nowak, Brett B. Palm, Jeff Peischl, Felix Piel, Pamela S. Rickly, Andrew W. Rollins, Thomas B. Ryerson, Rebecca H. Schwantes, Kanako Sekimoto, Lee Thornhill, Joel A. Thornton, Geoffrey S. Tyndall, Kirk Ullmann, Paul Van Rooy, Patrick R. Veres, Carsten Warneke, Rebecca A. Washenfelder, Andrew J. Weinheimer, Elizabeth Wiggins, Edward Winstead, Armin Wisthaler, Caroline Womack, and Steven S. Brown
Atmos. Chem. Phys., 21, 16293–16317, https://doi.org/10.5194/acp-21-16293-2021, https://doi.org/10.5194/acp-21-16293-2021, 2021
Short summary
Short summary
To understand air quality impacts from wildfires, we need an accurate picture of how wildfire smoke changes chemically both day and night as sunlight changes the chemistry of smoke. We present a chemical analysis of wildfire smoke as it changes from midday through the night. We use aircraft observations from the FIREX-AQ field campaign with a chemical box model. We find that even under sunlight typical
nighttimechemistry thrives and controls the fate of key smoke plume chemical processes.
Xuan Wang, Daniel J. Jacob, William Downs, Shuting Zhai, Lei Zhu, Viral Shah, Christopher D. Holmes, Tomás Sherwen, Becky Alexander, Mathew J. Evans, Sebastian D. Eastham, J. Andrew Neuman, Patrick R. Veres, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Thomas J. Bannan, Carl J. Percival, Ben H. Lee, and Joel A. Thornton
Atmos. Chem. Phys., 21, 13973–13996, https://doi.org/10.5194/acp-21-13973-2021, https://doi.org/10.5194/acp-21-13973-2021, 2021
Short summary
Short summary
Halogen radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a new mechanistic description and comprehensive simulation of tropospheric halogens in a global 3-D model and compare the model results with surface and aircraft measurements. We find that halogen chemistry decreases the global tropospheric burden of ozone by 11 %, NOx by 6 %, and OH by 4 %.
Emma Lumiaro, Milica Todorović, Theo Kurten, Hanna Vehkamäki, and Patrick Rinke
Atmos. Chem. Phys., 21, 13227–13246, https://doi.org/10.5194/acp-21-13227-2021, https://doi.org/10.5194/acp-21-13227-2021, 2021
Short summary
Short summary
The study of climate change relies on climate models, which require an understanding of aerosol formation. We train a machine-learning model to predict the partitioning coefficients of atmospheric molecules, which govern condensation into aerosols. The model can make instant predictions based on molecular structures with accuracy surpassing that of standard computational methods. This will allow the screening of low-volatility molecules that contribute most to aerosol formation.
Xiaolong Fan, Jing Cai, Chao Yan, Jian Zhao, Yishuo Guo, Chang Li, Kaspar R. Dällenbach, Feixue Zheng, Zhuohui Lin, Biwu Chu, Yonghong Wang, Lubna Dada, Qiaozhi Zha, Wei Du, Jenni Kontkanen, Theo Kurtén, Siddhart Iyer, Joni T. Kujansuu, Tuukka Petäjä, Douglas R. Worsnop, Veli-Matti Kerminen, Yongchun Liu, Federico Bianchi, Yee Jun Tham, Lei Yao, and Markku Kulmala
Atmos. Chem. Phys., 21, 11437–11452, https://doi.org/10.5194/acp-21-11437-2021, https://doi.org/10.5194/acp-21-11437-2021, 2021
Short summary
Short summary
We observed significant concentrations of gaseous HBr and HCl throughout the winter and springtime in urban Beijing, China. Our results indicate that gaseous HCl and HBr are most likely originated from anthropogenic emissions such as burning activities, and the gas–aerosol partitioning may play a crucial role in contributing to the gaseous HCl and HBr. These observations suggest that there is an important recycling pathway of halogen species in inland megacities.
Rongrong Wu, Luc Vereecken, Epameinondas Tsiligiannis, Sungah Kang, Sascha R. Albrecht, Luisa Hantschke, Defeng Zhao, Anna Novelli, Hendrik Fuchs, Ralf Tillmann, Thorsten Hohaus, Philip T. M. Carlsson, Justin Shenolikar, François Bernard, John N. Crowley, Juliane L. Fry, Bellamy Brownwood, Joel A. Thornton, Steven S. Brown, Astrid Kiendler-Scharr, Andreas Wahner, Mattias Hallquist, and Thomas F. Mentel
Atmos. Chem. Phys., 21, 10799–10824, https://doi.org/10.5194/acp-21-10799-2021, https://doi.org/10.5194/acp-21-10799-2021, 2021
Short summary
Short summary
Isoprene is the biogenic volatile organic compound with the largest emissions rates. The nighttime reaction of isoprene with the NO3 radical has a large potential to contribute to SOA. We classified isoprene nitrates into generations and proposed formation pathways. Considering the potential functionalization of the isoprene nitrates we propose that mainly isoprene dimers contribute to SOA formation from the isoprene NO3 reactions with at least a 5 % mass yield.
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.
Mingyi Wang, Xu-Cheng He, Henning Finkenzeller, Siddharth Iyer, Dexian Chen, Jiali Shen, Mario Simon, Victoria Hofbauer, Jasper Kirkby, Joachim Curtius, Norbert Maier, Theo Kurtén, Douglas R. Worsnop, Markku Kulmala, Matti Rissanen, Rainer Volkamer, Yee Jun Tham, Neil M. Donahue, and Mikko Sipilä
Atmos. Meas. Tech., 14, 4187–4202, https://doi.org/10.5194/amt-14-4187-2021, https://doi.org/10.5194/amt-14-4187-2021, 2021
Short summary
Short summary
Atmospheric iodine species are often short-lived with low abundance and have thus been challenging to measure. We show that the bromide chemical ionization mass spectrometry, compatible with both the atmospheric pressure and reduced pressure interfaces, can simultaneously detect various gas-phase iodine species. Combining calibration experiments and quantum chemical calculations, we quantify detection sensitivities to HOI, HIO3, I2, and H2SO4, giving detection limits down to < 106 molec. cm-3.
Jack J. Lin, Kamal Raj R Mundoli, Stella Wang, Esko Kokkonen, Mikko-Heikki Mikkelä, Samuli Urpelainen, and Nønne L. Prisle
Atmos. Chem. Phys., 21, 4709–4727, https://doi.org/10.5194/acp-21-4709-2021, https://doi.org/10.5194/acp-21-4709-2021, 2021
Short summary
Short summary
We used surface-sensitive X-ray photoelectron spectroscopy (XPS) to study laboratory-generated nanoparticles of atmospheric interest at 0–16 % relative humidity. XPS gives direct information about changes in the chemical state from the binding energies of probed elements. Our results indicate water adsorption and associated chemical changes at the particle surfaces well below deliquescence, with distinct features for different particle components and implications for atmospheric chemistry.
Georgia Michailoudi, Jack J. Lin, Hayato Yuzawa, Masanari Nagasaka, Marko Huttula, Nobuhiro Kosugi, Theo Kurtén, Minna Patanen, and Nønne L. Prisle
Atmos. Chem. Phys., 21, 2881–2894, https://doi.org/10.5194/acp-21-2881-2021, https://doi.org/10.5194/acp-21-2881-2021, 2021
Short summary
Short summary
This study provides insight into hydration of two significant atmospheric compounds, glyoxal and methylglyoxal. Using synchrotron radiation excited X-ray absorption spectroscopy, we confirm that glyoxal is fully hydrated in water, and for the first time, we experimentally detect enol structures in aqueous methylglyoxal. Our results support the contribution of these compounds to secondary organic aerosol formation, known to have a large uncertainty in atmospheric models and climate predictions.
Anna Shcherbacheva, Tracey Balehowsky, Jakub Kubečka, Tinja Olenius, Tapio Helin, Heikki Haario, Marko Laine, Theo Kurtén, and Hanna Vehkamäki
Atmos. Chem. Phys., 20, 15867–15906, https://doi.org/10.5194/acp-20-15867-2020, https://doi.org/10.5194/acp-20-15867-2020, 2020
Short summary
Short summary
Atmospheric new particle formation and cluster growth to aerosol particles is an important field of research, in particular due to the climate change phenomenon. Evaporation rates are very difficult to account for but they are important to explain the formation and growth of particles. Different quantum chemistry (QC) methods produce substantially different values for the evaporation rates. We propose a novel approach for inferring evaporation rates of clusters from available measurements.
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.
Yiqi Zheng, Joel A. Thornton, Nga Lee Ng, Hansen Cao, Daven K. Henze, Erin E. McDuffie, Weiwei Hu, Jose L. Jimenez, Eloise A. Marais, Eric Edgerton, and Jingqiu Mao
Atmos. Chem. Phys., 20, 13091–13107, https://doi.org/10.5194/acp-20-13091-2020, https://doi.org/10.5194/acp-20-13091-2020, 2020
Short summary
Short summary
This study aims to address a challenge in biosphere–atmosphere interactions: to what extent can biogenic organic aerosol (OA) be modified through human activities? From three surface network observations, we show OA is weakly dependent on sulfate and aerosol acidity in the summer southeast US, on both long-term trends and monthly variability. The results are in strong contrast to a global model, GEOS-Chem, suggesting the need to revisit the representation of aqueous-phase secondary OA formation.
Ryan Schmedding, Quazi Z. Rasool, Yue Zhang, Havala O. T. Pye, Haofei Zhang, Yuzhi Chen, Jason D. Surratt, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Allen H. Goldstein, and William Vizuete
Atmos. Chem. Phys., 20, 8201–8225, https://doi.org/10.5194/acp-20-8201-2020, https://doi.org/10.5194/acp-20-8201-2020, 2020
Short summary
Short summary
Accurate model prediction of aerosol concentrations is a known challenge. It is assumed in many modeling systems that aerosols are in a homogeneously mixed phase state. It has been observed that aerosols do phase separate and can form a highly viscous organic shell with an aqueous core impacting the formation processes of aerosols. This work is a model implementation to determine an aerosol's phase state using glass transition temperature and aerosol composition.
Tommaso Zanca, Jakub Kubečka, Evgeni Zapadinsky, Monica Passananti, Theo Kurtén, and Hanna Vehkamäki
Atmos. Meas. Tech., 13, 3581–3593, https://doi.org/10.5194/amt-13-3581-2020, https://doi.org/10.5194/amt-13-3581-2020, 2020
Short summary
Short summary
In this paper we quantify (using a statistical model) the probability of decomposition of a representative class of HOM clusters in an APi-TOF mass spectrometer. This is important because it quantifies the systematic error of measurements in a APi-TOF MS due to cluster decomposition. The results (specific for our selected clusters) show that decomposition is negligible, provided their bonding energy is large enough to allow formation in the atmosphere in the first place.
Noora Hyttinen, Jonas Elm, Jussi Malila, Silvia M. Calderón, and Nønne L. Prisle
Atmos. Chem. Phys., 20, 5679–5696, https://doi.org/10.5194/acp-20-5679-2020, https://doi.org/10.5194/acp-20-5679-2020, 2020
Short summary
Short summary
Organosulfates have been identified in atmospheric secondary organic aerosol (SOA). The thermodynamic properties of SOA constituents, such as organosulfates, affect the stability and atmospheric impact of the SOA. Here we present estimated solubility, activity, pKa, saturation vapor pressure and Henry's law solubility values for several atmospherically relevant monoterpene- and isoprene-derived organosulfate compounds. These properties can be used, for example, in aerosol process modeling.
Ziyue Li, Emma L. D'Ambro, Siegfried Schobesberger, Cassandra J. Gaston, Felipe D. Lopez-Hilfiker, Jiumeng Liu, John E. Shilling, Joel A. Thornton, and Christopher D. Cappa
Atmos. Chem. Phys., 20, 2489–2512, https://doi.org/10.5194/acp-20-2489-2020, https://doi.org/10.5194/acp-20-2489-2020, 2020
Short summary
Short summary
We discuss the development and application of a robust clustering method for the interpretation of compound-specific organic aerosol thermal desorption profiles. We demonstrate the utility of clustering for analysis and interpretation of the composition and volatility of secondary organic aerosol. We show that the thermal desorption profiles are represented by only 9–13 distinct clusters, with the number of clusters obtained dependent on the precursor and formation conditions.
Brett B. Palm, Xiaoxi Liu, Jose L. Jimenez, and Joel A. Thornton
Atmos. Meas. Tech., 12, 5829–5844, https://doi.org/10.5194/amt-12-5829-2019, https://doi.org/10.5194/amt-12-5829-2019, 2019
Short summary
Short summary
We introduce a coaxial, low-pressure ion–molecule reaction (IMR) region for iodide-adduct chemical ionization mass spectrometry, designed to decrease the effects of IMR wall interactions with organic/inorganic gases. This IMR has 3–10 times shorter delay times than previous IMRs. We introduce a conceptual framework for understanding and subtracting the background signal due to analyte molecules interacting with IMR walls. This framework can be applied to other tubing and instrument systems.
Roope Halonen, Evgeni Zapadinsky, Theo Kurtén, Hanna Vehkamäki, and Bernhard Reischl
Atmos. Chem. Phys., 19, 13355–13366, https://doi.org/10.5194/acp-19-13355-2019, https://doi.org/10.5194/acp-19-13355-2019, 2019
Short summary
Short summary
The rate of collisions between molecules or clusters is used to determine particle formation in the atmosphere. The basic approach is to treat the colliding particles as noninteracting hard spheres. By using atomistic simulations with a realistic force field and theoretical approaches, we showed that the actual collision rate of two sulfuric acid molecules is more than twice as high as that for hard spheres. The results of this study will improve models of atmospheric particle growth.
Felipe D. Lopez-Hilfiker, Veronika Pospisilova, Wei Huang, Markus Kalberer, Claudia Mohr, Giulia Stefenelli, Joel A. Thornton, Urs Baltensperger, Andre S. H. Prevot, and Jay G. Slowik
Atmos. Meas. Tech., 12, 4867–4886, https://doi.org/10.5194/amt-12-4867-2019, https://doi.org/10.5194/amt-12-4867-2019, 2019
Short summary
Short summary
We present a novel, field-deployable extractive electrospray time-of-flight mass spectrometer (EESI-TOF), which provides real-time, near-molecular measurements of organic aerosol at atmospherically relevant concentrations, addressing a critical gap in existing measurement capabilities. Successful deployments of the EESI-TOF for laboratory measurements, ground-based ambient sampling, and aboard a research aircraft highlight the versatility and potential of the EESI-TOF system.
Emma L. D'Ambro, Siegfried Schobesberger, Cassandra J. Gaston, Felipe D. Lopez-Hilfiker, Ben H. Lee, Jiumeng Liu, Alla Zelenyuk, David Bell, Christopher D. Cappa, Taylor Helgestad, Ziyue Li, Alex Guenther, Jian Wang, Matthew Wise, Ryan Caylor, Jason D. Surratt, Theran Riedel, Noora Hyttinen, Vili-Taneli Salo, Galib Hasan, Theo Kurtén, John E. Shilling, and Joel A. Thornton
Atmos. Chem. Phys., 19, 11253–11265, https://doi.org/10.5194/acp-19-11253-2019, https://doi.org/10.5194/acp-19-11253-2019, 2019
Short summary
Short summary
Isoprene is the most abundantly emitted reactive organic gas globally, and thus it is important to understand its fate and role in aerosol formation and growth. A major product of its oxidation is an epoxydiol, IEPOX, which can be efficiently taken up by acidic aerosol to generate substantial amounts of secondary organic aerosol (SOA). We present chamber experiments exploring the properties of IEPOX SOA and reconcile discrepancies between field, laboratory, and model studies of this process.
Erin E. McDuffie, Caroline C. Womack, Dorothy L. Fibiger, William P. Dube, Alessandro Franchin, Ann M. Middlebrook, Lexie Goldberger, Ben H. Lee, Joel A. Thornton, Alexander Moravek, Jennifer G. Murphy, Munkhbayar Baasandorj, and Steven S. Brown
Atmos. Chem. Phys., 19, 9287–9308, https://doi.org/10.5194/acp-19-9287-2019, https://doi.org/10.5194/acp-19-9287-2019, 2019
Short summary
Short summary
Populated mountain basins, including the Salt Lake Valley (SLV) in Utah, suffer from wintertime stagnation events that trap emissions near the surface and cause fine particulate matter (PM2.5) concentrations to reach unhealthy levels. Previously limited by a lack of nighttime measurements, this study uses 2017 UWFPS aircraft campaign data, in combination with a box model, to show that nitrogen chemistry above the surface at night is a major source of PM2.5 during a wintertime event in the SLV.
Xiaoxi Liu, Benjamin Deming, Demetrios Pagonis, Douglas A. Day, Brett B. Palm, Ranajit Talukdar, James M. Roberts, Patrick R. Veres, Jordan E. Krechmer, Joel A. Thornton, Joost A. de Gouw, Paul J. Ziemann, and Jose L. Jimenez
Atmos. Meas. Tech., 12, 3137–3149, https://doi.org/10.5194/amt-12-3137-2019, https://doi.org/10.5194/amt-12-3137-2019, 2019
Short summary
Short summary
Delays or losses of gases in sampling tubing and instrumental surfaces due to surface interactions can lead to inaccurate quantification. By sampling with several chemical ionization mass spectrometers and six tubing materials, we quantify delays of semivolatile organic compounds and small polar gases. Delay times generally increase with decreasing volatility or increasing polarity and also depend on materials. The method and results will inform inlet material selection and instrumental design.
Nønne L. Prisle, Jack J. Lin, Sara Purdue, Haisheng Lin, J. Carson Meredith, and Athanasios Nenes
Atmos. Chem. Phys., 19, 4741–4761, https://doi.org/10.5194/acp-19-4741-2019, https://doi.org/10.5194/acp-19-4741-2019, 2019
Short summary
Short summary
We measure surface activity and cloud-forming potential of pollenkitt, an organic mixture coating pollen grains. Cloud droplet formation is affected through both surface tension and bulk depletion, with a consistent particle size-dependent signature. We observe nonideal solution effects in pollenkitt mixtures with ammonium sulfate salt. Our results suggest sensitivity of general water interactions, including cloud formation by pollen and their fragments, to both atmospheric humidity and aging.
Xuan Wang, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Lei Zhu, Qianjie Chen, Becky Alexander, Tomás Sherwen, Mathew J. Evans, Ben H. Lee, Jessica D. Haskins, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Gregory L. Huey, and Hong Liao
Atmos. Chem. Phys., 19, 3981–4003, https://doi.org/10.5194/acp-19-3981-2019, https://doi.org/10.5194/acp-19-3981-2019, 2019
Short summary
Short summary
Chlorine radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a comprehensive simulation of tropospheric chlorine in a global 3-D model, which includes explicit accounting of chloride mobilization from sea salt aerosol. We find the chlorine chemistry contributes 1.0 % of the global oxidation of methane and decreases global burdens of tropospheric ozone by 7 % and OH by 3 % through the associated bromine radical chemistry.
Michael Boy, Erik S. Thomson, Juan-C. Acosta Navarro, Olafur Arnalds, Ekaterina Batchvarova, Jaana Bäck, Frank Berninger, Merete Bilde, Zoé Brasseur, Pavla Dagsson-Waldhauserova, Dimitri Castarède, Maryam Dalirian, Gerrit de Leeuw, Monika Dragosics, Ella-Maria Duplissy, Jonathan Duplissy, Annica M. L. Ekman, Keyan Fang, Jean-Charles Gallet, Marianne Glasius, Sven-Erik Gryning, Henrik Grythe, Hans-Christen Hansson, Margareta Hansson, Elisabeth Isaksson, Trond Iversen, Ingibjorg Jonsdottir, Ville Kasurinen, Alf Kirkevåg, Atte Korhola, Radovan Krejci, Jon Egill Kristjansson, Hanna K. Lappalainen, Antti Lauri, Matti Leppäranta, Heikki Lihavainen, Risto Makkonen, Andreas Massling, Outi Meinander, E. Douglas Nilsson, Haraldur Olafsson, Jan B. C. Pettersson, Nønne L. Prisle, Ilona Riipinen, Pontus Roldin, Meri Ruppel, Matthew Salter, Maria Sand, Øyvind Seland, Heikki Seppä, Henrik Skov, Joana Soares, Andreas Stohl, Johan Ström, Jonas Svensson, Erik Swietlicki, Ksenia Tabakova, Throstur Thorsteinsson, Aki Virkkula, Gesa A. Weyhenmeyer, Yusheng Wu, Paul Zieger, and Markku Kulmala
Atmos. Chem. Phys., 19, 2015–2061, https://doi.org/10.5194/acp-19-2015-2019, https://doi.org/10.5194/acp-19-2015-2019, 2019
Short summary
Short summary
The Nordic Centre of Excellence CRAICC (Cryosphere–Atmosphere Interactions in a Changing Arctic Climate), funded by NordForsk in the years 2011–2016, is the largest joint Nordic research and innovation initiative to date and aimed to strengthen research and innovation regarding climate change issues in the Nordic region. The paper presents an overview of the main scientific topics investigated and provides a state-of-the-art comprehensive summary of what has been achieved in CRAICC.
Alessandro Franchin, Dorothy L. Fibiger, Lexie Goldberger, Erin E. McDuffie, Alexander Moravek, Caroline C. Womack, Erik T. Crosman, Kenneth S. Docherty, William P. Dube, Sebastian W. Hoch, Ben H. Lee, Russell Long, Jennifer G. Murphy, Joel A. Thornton, Steven S. Brown, Munkhbayar Baasandorj, and Ann M. Middlebrook
Atmos. Chem. Phys., 18, 17259–17276, https://doi.org/10.5194/acp-18-17259-2018, https://doi.org/10.5194/acp-18-17259-2018, 2018
Short summary
Short summary
We present the results of aerosol and trace gas measurements from airborne and ground-based platforms. The measurements took place in January–February 2017 in northern Utah as part of the Utah Winter Fine Particulate Study (UWFPS). We characterized the chemical composition of PM1 on a regional scale, also probing the vertical dimension. We used a thermodynamic model to study the effectiveness of limiting total ammonium or total nitrate as a strategy to control aerosol concentrations.
Siegfried Schobesberger, Emma L. D'Ambro, Felipe D. Lopez-Hilfiker, Claudia Mohr, and Joel A. Thornton
Atmos. Chem. Phys., 18, 14757–14785, https://doi.org/10.5194/acp-18-14757-2018, https://doi.org/10.5194/acp-18-14757-2018, 2018
Short summary
Short summary
Current mass spectrometers allow us to measure the composition of individual organic molecules in aerosol particles, as well as how they evaporate from the particles when those are slowly heated up to 200 °C. We have developed a detailed computer model to simulate the physical and chemical processes that underlie that evaporation and thus help us understand important aerosol properties. Among other factors, we discuss the roles of vapor pressures, and accretion and decomposition reactions.
Ben H. Lee, Felipe D. Lopez-Hilfiker, Emma L. D'Ambro, Putian Zhou, Michael Boy, Tuukka Petäjä, Liqing Hao, Annele Virtanen, and Joel A. Thornton
Atmos. Chem. Phys., 18, 11547–11562, https://doi.org/10.5194/acp-18-11547-2018, https://doi.org/10.5194/acp-18-11547-2018, 2018
Short summary
Short summary
Molecular identities and abundances of organic compounds residing in the gas and particle phases above a Finnish boreal forest are presented. We determined that in each phase, the organic components are categorized into three subgroups based on their behavior in time. Some are more enhanced at night, others during midday, and another around sunrise. Identifying such collective behavior can potentially connect the chemical processes that evolve in time to specific distributions of products.
Jingyi Li, Jingqiu Mao, Arlene M. Fiore, Ronald C. Cohen, John D. Crounse, Alex P. Teng, Paul O. Wennberg, Ben H. Lee, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Jeff Peischl, Ilana B. Pollack, Thomas B. Ryerson, Patrick Veres, James M. Roberts, J. Andrew Neuman, John B. Nowak, Glenn M. Wolfe, Thomas F. Hanisco, Alan Fried, Hanwant B. Singh, Jack Dibb, Fabien Paulot, and Larry W. Horowitz
Atmos. Chem. Phys., 18, 2341–2361, https://doi.org/10.5194/acp-18-2341-2018, https://doi.org/10.5194/acp-18-2341-2018, 2018
Short summary
Short summary
We present the first comprehensive model evaluation of summertime reactive oxidized nitrogen using a high-resolution chemistry–climate model with up-to-date isoprene oxidation chemistry, along with a series of observations from aircraft campaigns and ground measurement networks from 2004 to 2013 over the Southeast US. We investigate the impact of NOx emission reductions on changes in reactive nitrogen speciation and export efficiency as well as ozone in the past and future decade.
Ulrich K. Krieger, Franziska Siegrist, Claudia Marcolli, Eva U. Emanuelsson, Freya M. Gøbel, Merete Bilde, Aleksandra Marsh, Jonathan P. Reid, Andrew J. Huisman, Ilona Riipinen, Noora Hyttinen, Nanna Myllys, Theo Kurtén, Thomas Bannan, Carl J. Percival, and David Topping
Atmos. Meas. Tech., 11, 49–63, https://doi.org/10.5194/amt-11-49-2018, https://doi.org/10.5194/amt-11-49-2018, 2018
Short summary
Short summary
Vapor pressures of low-volatility organic molecules at atmospheric temperatures reported in the literature often differ by several orders of magnitude between measurement techniques. These discrepancies exceed the stated uncertainty of each technique, which is generally reported to be smaller than a factor of 2. We determined saturation vapor pressures for the homologous series of polyethylene glycols ranging in vapor pressure at 298 K from 1E−7 Pa to 5E−2 Pa as a reference set.
Yue Zhao, Jeremy K. Chan, Felipe D. Lopez-Hilfiker, Megan A. McKeown, Emma L. D'Ambro, Jay G. Slowik, Jeffrey A. Riffell, and Joel A. Thornton
Atmos. Meas. Tech., 10, 3609–3625, https://doi.org/10.5194/amt-10-3609-2017, https://doi.org/10.5194/amt-10-3609-2017, 2017
Short summary
Short summary
We present a novel atmospheric pressure electrospray chemical ionization (ESCI) source that can generate intense and stable currents of several specific reagent ions using a range of salt solutions prepared in methanol. We couple the ESCI source to a high-resolution time-of-flight mass spectrometer (HRToF-MS) and assess instrument performance through calibrations using different gas standards and measurements of organic mixtures formed by ozonolysis of α-pinene.
Emilie Öström, Zhou Putian, Guy Schurgers, Mikhail Mishurov, Niku Kivekäs, Heikki Lihavainen, Mikael Ehn, Matti P. Rissanen, Theo Kurtén, Michael Boy, Erik Swietlicki, and Pontus Roldin
Atmos. Chem. Phys., 17, 8887–8901, https://doi.org/10.5194/acp-17-8887-2017, https://doi.org/10.5194/acp-17-8887-2017, 2017
Short summary
Short summary
We used a model to study how biogenic volatile organic compounds (BVOCs) emitted from the boreal forest contribute to the formation and growth of particles in the atmosphere. Some of these particles are important climate forcers, acting as seeds for cloud droplet fomation. We implemented a new gas chemistry mechanism that describes how the BVOCs are oxidized and form low-volatility highly oxidized organic molecules. With the new mechanism we are able to accurately predict the particle growth.
Juan Hong, Mikko Äijälä, Silja A. K. Häme, Liqing Hao, Jonathan Duplissy, Liine M. Heikkinen, Wei Nie, Jyri Mikkilä, Markku Kulmala, Nønne L. Prisle, Annele Virtanen, Mikael Ehn, Pauli Paasonen, Douglas R. Worsnop, Ilona Riipinen, Tuukka Petäjä, and Veli-Matti Kerminen
Atmos. Chem. Phys., 17, 4387–4399, https://doi.org/10.5194/acp-17-4387-2017, https://doi.org/10.5194/acp-17-4387-2017, 2017
Short summary
Short summary
Estimates of volatility of secondary organic aerosols was characterized in a boreal forest environment of Hyytiälä, southern Finland. This was done by interpreting field measurements using a volatility tandem differential mobility analyzer (VTDMA) with a kinetic evaporation model and by applying positive matrix factorization (PMF) to high-resolution aerosol mass spectrometer data. About 16 % of the variation can be explained by the linear regression between the results from these two methods.
Nga Lee Ng, Steven S. Brown, Alexander T. Archibald, Elliot Atlas, Ronald C. Cohen, John N. Crowley, Douglas A. Day, Neil M. Donahue, Juliane L. Fry, Hendrik Fuchs, Robert J. Griffin, Marcelo I. Guzman, Hartmut Herrmann, Alma Hodzic, Yoshiteru Iinuma, José L. Jimenez, Astrid Kiendler-Scharr, Ben H. Lee, Deborah J. Luecken, Jingqiu Mao, Robert McLaren, Anke Mutzel, Hans D. Osthoff, Bin Ouyang, Benedicte Picquet-Varrault, Ulrich Platt, Havala O. T. Pye, Yinon Rudich, Rebecca H. Schwantes, Manabu Shiraiwa, Jochen Stutz, Joel A. Thornton, Andreas Tilgner, Brent J. Williams, and Rahul A. Zaveri
Atmos. Chem. Phys., 17, 2103–2162, https://doi.org/10.5194/acp-17-2103-2017, https://doi.org/10.5194/acp-17-2103-2017, 2017
Short summary
Short summary
Oxidation of biogenic volatile organic compounds by NO3 is an important interaction between anthropogenic
and natural emissions. This review results from a June 2015 workshop and includes the recent literature
on kinetics, mechanisms, organic aerosol yields, and heterogeneous chemistry; advances in analytical
instrumentation; the current state NO3-BVOC chemistry in atmospheric models; and critical needs for
future research in modeling, field observations, and laboratory studies.
Emma L. D'Ambro, Ben H. Lee, Jiumeng Liu, John E. Shilling, Cassandra J. Gaston, Felipe D. Lopez-Hilfiker, Siegfried Schobesberger, Rahul A. Zaveri, Claudia Mohr, Anna Lutz, Zhenfa Zhang, Avram Gold, Jason D. Surratt, Jean C. Rivera-Rios, Frank N. Keutsch, and Joel A. Thornton
Atmos. Chem. Phys., 17, 159–174, https://doi.org/10.5194/acp-17-159-2017, https://doi.org/10.5194/acp-17-159-2017, 2017
Short summary
Short summary
We studied the formation and properties of secondary organic aerosol produced from isoprene. We find that a significant fraction (~50 %) of the mass is composed of low-volatility, highly oxidized compounds such as C5H12O6. A significant fraction of the remainder appears to be in the form of oligomeric material. Adding NOx maintained or decreased SOA yields while increasing the fraction of low-volatility material, possibly due to oligomers.
Hanna K. Lappalainen, Veli-Matti Kerminen, Tuukka Petäjä, Theo Kurten, Aleksander Baklanov, Anatoly Shvidenko, Jaana Bäck, Timo Vihma, Pavel Alekseychik, Meinrat O. Andreae, Stephen R. Arnold, Mikhail Arshinov, Eija Asmi, Boris Belan, Leonid Bobylev, Sergey Chalov, Yafang Cheng, Natalia Chubarova, Gerrit de Leeuw, Aijun Ding, Sergey Dobrolyubov, Sergei Dubtsov, Egor Dyukarev, Nikolai Elansky, Kostas Eleftheriadis, Igor Esau, Nikolay Filatov, Mikhail Flint, Congbin Fu, Olga Glezer, Aleksander Gliko, Martin Heimann, Albert A. M. Holtslag, Urmas Hõrrak, Juha Janhunen, Sirkku Juhola, Leena Järvi, Heikki Järvinen, Anna Kanukhina, Pavel Konstantinov, Vladimir Kotlyakov, Antti-Jussi Kieloaho, Alexander S. Komarov, Joni Kujansuu, Ilmo Kukkonen, Ella-Maria Duplissy, Ari Laaksonen, Tuomas Laurila, Heikki Lihavainen, Alexander Lisitzin, Alexsander Mahura, Alexander Makshtas, Evgeny Mareev, Stephany Mazon, Dmitry Matishov, Vladimir Melnikov, Eugene Mikhailov, Dmitri Moisseev, Robert Nigmatulin, Steffen M. Noe, Anne Ojala, Mari Pihlatie, Olga Popovicheva, Jukka Pumpanen, Tatjana Regerand, Irina Repina, Aleksei Shcherbinin, Vladimir Shevchenko, Mikko Sipilä, Andrey Skorokhod, Dominick V. Spracklen, Hang Su, Dmitry A. Subetto, Junying Sun, Arkady Y. Terzhevik, Yuri Timofeyev, Yuliya Troitskaya, Veli-Pekka Tynkkynen, Viacheslav I. Kharuk, Nina Zaytseva, Jiahua Zhang, Yrjö Viisanen, Timo Vesala, Pertti Hari, Hans Christen Hansson, Gennady G. Matvienko, Nikolai S. Kasimov, Huadong Guo, Valery Bondur, Sergej Zilitinkevich, and Markku Kulmala
Atmos. Chem. Phys., 16, 14421–14461, https://doi.org/10.5194/acp-16-14421-2016, https://doi.org/10.5194/acp-16-14421-2016, 2016
Short summary
Short summary
After kick off in 2012, the Pan-Eurasian Experiment (PEEX) program has expanded fast and today the multi-disciplinary research community covers ca. 80 institutes and a network of ca. 500 scientists from Europe, Russia, and China. Here we introduce scientific topics relevant in this context. This is one of the first multi-disciplinary overviews crossing scientific boundaries, from atmospheric sciences to socio-economics and social sciences.
Neha Sareen, Annmarie G. Carlton, Jason D. Surratt, Avram Gold, Ben Lee, Felipe D. Lopez-Hilfiker, Claudia Mohr, Joel A. Thornton, Zhenfa Zhang, Yong B. Lim, and Barbara J. Turpin
Atmos. Chem. Phys., 16, 14409–14420, https://doi.org/10.5194/acp-16-14409-2016, https://doi.org/10.5194/acp-16-14409-2016, 2016
Carsten Warneke, Michael Trainer, Joost A. de Gouw, David D. Parrish, David W. Fahey, A. R. Ravishankara, Ann M. Middlebrook, Charles A. Brock, James M. Roberts, Steven S. Brown, Jonathan A. Neuman, Brian M. Lerner, Daniel Lack, Daniel Law, Gerhard Hübler, Iliana Pollack, Steven Sjostedt, Thomas B. Ryerson, Jessica B. Gilman, Jin Liao, John Holloway, Jeff Peischl, John B. Nowak, Kenneth C. Aikin, Kyung-Eun Min, Rebecca A. Washenfelder, Martin G. Graus, Mathew Richardson, Milos Z. Markovic, Nick L. Wagner, André Welti, Patrick R. Veres, Peter Edwards, Joshua P. Schwarz, Timothy Gordon, William P. Dube, Stuart A. McKeen, Jerome Brioude, Ravan Ahmadov, Aikaterini Bougiatioti, Jack J. Lin, Athanasios Nenes, Glenn M. Wolfe, Thomas F. Hanisco, Ben H. Lee, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Frank N. Keutsch, Jennifer Kaiser, Jingqiu Mao, and Courtney D. Hatch
Atmos. Meas. Tech., 9, 3063–3093, https://doi.org/10.5194/amt-9-3063-2016, https://doi.org/10.5194/amt-9-3063-2016, 2016
Short summary
Short summary
In this paper we describe the experimental approach, the science goals and early results of the NOAA SENEX campaign, which was focused on studying the interactions between biogenic and anthropogenic emissions to form secondary pollutants.
During SENEX, the NOAA WP-3D aircraft conducted 20 research flights between 27 May and 10 July 2013 based out of Smyrna, TN. The SENEX flights included day- and nighttime flights in the Southeast as well as flights over areas with intense shale gas extraction.
Felipe D. Lopez-Hilfiker, Siddarth Iyer, Claudia Mohr, Ben H. Lee, Emma L. D'Ambro, Theo Kurtén, and Joel A. Thornton
Atmos. Meas. Tech., 9, 1505–1512, https://doi.org/10.5194/amt-9-1505-2016, https://doi.org/10.5194/amt-9-1505-2016, 2016
Short summary
Short summary
We present the maximum sensitivity of a TOF-CIMS using the collision limit and iodide adducts. We also present an ion adduct declustering scanning procedure which determines the effective binding energies of the detected ion adducts and therefore their approximate sensitivity. The combination of declustering scanning and the collision limit provides an approximate calibration for many compounds in the mass spectrum which would otherwise be impossible to obtain by traditional methods.
G. M. Wolfe, J. Kaiser, T. F. Hanisco, F. N. Keutsch, J. A. de Gouw, J. B. Gilman, M. Graus, C. D. Hatch, J. Holloway, L. W. Horowitz, B. H. Lee, B. M. Lerner, F. Lopez-Hilifiker, J. Mao, M. R. Marvin, J. Peischl, I. B. Pollack, J. M. Roberts, T. B. Ryerson, J. A. Thornton, P. R. Veres, and C. Warneke
Atmos. Chem. Phys., 16, 2597–2610, https://doi.org/10.5194/acp-16-2597-2016, https://doi.org/10.5194/acp-16-2597-2016, 2016
Short summary
Short summary
This study uses airborne trace gas observations acquired over the southeast US to examine how both natural (isoprene) and anthropogenic (NOx) emissions influence the production of formaldehyde (HCHO). We find a 3-fold increase in HCHO yield between rural and polluted environments. State-of-the-science chemical mechanisms are generally able to reproduce this behavior. These results add confidence to global hydrocarbon emission inventories constrained by spaceborne HCHO observations.
Bjarke Mølgaard, Jarno Vanhatalo, Pasi P. Aalto, Nønne L. Prisle, and Kaarle Hämeri
Atmos. Meas. Tech., 9, 741–751, https://doi.org/10.5194/amt-9-741-2016, https://doi.org/10.5194/amt-9-741-2016, 2016
Short summary
Short summary
We have improved the reliability of submicron aerosol particle size distributions measured in urban locations. This improvement was obtained by processing the data in a new way and avoiding a problematic assumption of a stationary aerosol during each size distribution measurement.
T. P. Riedel, Y.-H. Lin, Z. Zhang, K. Chu, J. A. Thornton, W. Vizuete, A. Gold, and J. D. Surratt
Atmos. Chem. Phys., 16, 1245–1254, https://doi.org/10.5194/acp-16-1245-2016, https://doi.org/10.5194/acp-16-1245-2016, 2016
Short summary
Short summary
IEPOX, a photooxidation product of isoprene, contributes to ambient secondary organic aerosol concentrations. Controlled atmospheric chamber experiments and modeling are used to extract formation rate information of chemical species that contribute to IEPOX-derived secondary organic aerosol.
R. J. Wild, P. M. Edwards, T. S. Bates, R. C. Cohen, J. A. de Gouw, W. P. Dubé, J. B. Gilman, J. Holloway, J. Kercher, A. R. Koss, L. Lee, B. M. Lerner, R. McLaren, P. K. Quinn, J. M. Roberts, J. Stutz, J. A. Thornton, P. R. Veres, C. Warneke, E. Williams, C. J. Young, B. Yuan, K. J. Zarzana, and S. S. Brown
Atmos. Chem. Phys., 16, 573–583, https://doi.org/10.5194/acp-16-573-2016, https://doi.org/10.5194/acp-16-573-2016, 2016
Short summary
Short summary
High wintertime ozone levels have been observed in the Uintah Basin, Utah, a sparsely populated rural region with intensive oil and gas operations. The reactive nitrogen budget plays an important role in tropospheric ozone formation, and we find that nighttime chemistry has a large effect on its partitioning. Much of the oxidation of reactive nitrogen during a high-ozone year occurred via heterogeneous uptake onto aerosol at night, keeping NOx at concentrations comparable to a low-ozone year.
M. Kulmala, H. K. Lappalainen, T. Petäjä, T. Kurten, V.-M. Kerminen, Y. Viisanen, P. Hari, S. Sorvari, J. Bäck, V. Bondur, N. Kasimov, V. Kotlyakov, G. Matvienko, A. Baklanov, H. D. Guo, A. Ding, H.-C. Hansson, and S. Zilitinkevich
Atmos. Chem. Phys., 15, 13085–13096, https://doi.org/10.5194/acp-15-13085-2015, https://doi.org/10.5194/acp-15-13085-2015, 2015
Short summary
Short summary
The Pan-European Experiment (PEEX) is introduced. PEEX is a multidisciplinary, multiscale and multicomponent research, research infrastructure and capacity-building program. This paper outlines the mission, vision and objectives of PEEX and introduces its main components, including the research agenda, research infrastructure, knowledge transfer and potential impacts on society. The paper also summarizes the main scientific questions that PEEX is going to tackle in the future.
F. D. Lopez-Hilfiker, C. Mohr, M. Ehn, F. Rubach, E. Kleist, J. Wildt, Th. F. Mentel, A. J. Carrasquillo, K. E. Daumit, J. F. Hunter, J. H. Kroll, D. R. Worsnop, and J. A. Thornton
Atmos. Chem. Phys., 15, 7765–7776, https://doi.org/10.5194/acp-15-7765-2015, https://doi.org/10.5194/acp-15-7765-2015, 2015
Short summary
Short summary
We measured a large suite organic compounds using a recently developed Filter Inlet for Gases and AEROsols (FIGAERO) coupled to a (HR-ToF-CIMS). The instrument was deployed on environmental simulation chambers to study monoterpene oxidation as a secondary organic aerosol (SOA) source. We find that approximately 50% of the detected particle phase mass is associated with compounds having effective vapor pressures 4, or more, orders of magnitude lower than commonly measured products.
K. Ruusuvuori, P. Hietala, O. Kupiainen-Määttä, T. Jokinen, H. Junninen, M. Sipilä, T. Kurtén, and H. Vehkamäki
Atmos. Meas. Tech., 8, 2577–2588, https://doi.org/10.5194/amt-8-2577-2015, https://doi.org/10.5194/amt-8-2577-2015, 2015
Short summary
Short summary
Ionization reagents suitable for accurate measurements of the atmospheric gas-phase amine vapour concentrations are needed. Based on computational results, acetone is a viable option for use as an ionization reagent in CI-APi-TOF measurements on atmospheric dimethylamine. However, comparison between the computational and experimental results revealed notable discrepancies. Further study is still required before the acetone CI-APi-TOF can be considered a viable option in practice.
T. F. Mentel, M. Springer, M. Ehn, E. Kleist, I. Pullinen, T. Kurtén, M. Rissanen, A. Wahner, and J. Wildt
Atmos. Chem. Phys., 15, 6745–6765, https://doi.org/10.5194/acp-15-6745-2015, https://doi.org/10.5194/acp-15-6745-2015, 2015
Short summary
Short summary
We studied a series of cycloalkenes and methyl-substituted alkenes in order to elucidate the structural pre-requisites and chemical pathways to the recently discovered class of highly oxidized molecules ELVOC (Ehn et al., Nature, 2014). ELVOC may totally change the view on (parts of) the mechanism of SOA formation. We present results which support recent observations of H shifts from C-H to peroxy radicals, highlighting the pivotal role of peroxyradicals in organic atmospheric chemistry.
D. B. Millet, M. Baasandorj, D. K. Farmer, J. A. Thornton, K. Baumann, P. Brophy, S. Chaliyakunnel, J. A. de Gouw, M. Graus, L. Hu, A. Koss, B. H. Lee, F. D. Lopez-Hilfiker, J. A. Neuman, F. Paulot, J. Peischl, I. B. Pollack, T. B. Ryerson, C. Warneke, B. J. Williams, and J. Xu
Atmos. Chem. Phys., 15, 6283–6304, https://doi.org/10.5194/acp-15-6283-2015, https://doi.org/10.5194/acp-15-6283-2015, 2015
Short summary
Short summary
Formic acid (HCOOH) is an abundant atmospheric acid that affects precipitation chemistry and acidity. HCOOH measurements over the USA are 2-3× larger than can be explained by known sources and sinks, revealing a key gap in current understanding. Observations indicate a large biogenic source plus chemical production across a range of precursors. Model simulations cannot capture the HCOOH diurnal amplitude or nocturnal profile, implying a deposition bias and possibly even larger missing source.
H. Vuollekoski, M. Vogt, V. A. Sinclair, J. Duplissy, H. Järvinen, E.-M. Kyrö, R. Makkonen, T. Petäjä, N. L. Prisle, P. Räisänen, M. Sipilä, J. Ylhäisi, and M. Kulmala
Hydrol. Earth Syst. Sci., 19, 601–613, https://doi.org/10.5194/hess-19-601-2015, https://doi.org/10.5194/hess-19-601-2015, 2015
Short summary
Short summary
The global potential for collecting usable water from dew on an
artificial collector sheet was investigated by utilising 34 years of
meteorological reanalysis data as input to a dew formation model. Continental dew formation was found to be frequent and common, but daily yields were
mostly below 0.1mm.
M. Sipilä, T. Jokinen, T. Berndt, S. Richters, R. Makkonen, N. M. Donahue, R. L. Mauldin III, T. Kurtén, P. Paasonen, N. Sarnela, M. Ehn, H. Junninen, M. P. Rissanen, J. Thornton, F. Stratmann, H. Herrmann, D. R. Worsnop, M. Kulmala, V.-M. Kerminen, and T. Petäjä
Atmos. Chem. Phys., 14, 12143–12153, https://doi.org/10.5194/acp-14-12143-2014, https://doi.org/10.5194/acp-14-12143-2014, 2014
I. K. Ortega, T. Olenius, O. Kupiainen-Määttä, V. Loukonen, T. Kurtén, and H. Vehkamäki
Atmos. Chem. Phys., 14, 7995–8007, https://doi.org/10.5194/acp-14-7995-2014, https://doi.org/10.5194/acp-14-7995-2014, 2014
C. J. Gaston, J. A. Thornton, and N. L. Ng
Atmos. Chem. Phys., 14, 5693–5707, https://doi.org/10.5194/acp-14-5693-2014, https://doi.org/10.5194/acp-14-5693-2014, 2014
S. Bleicher, J. C. Buxmann, R. Sander, T. P. Riedel, J. A. Thornton, U. Platt, and C. Zetzsch
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-14-10135-2014, https://doi.org/10.5194/acpd-14-10135-2014, 2014
Revised manuscript has not been submitted
T. P. Riedel, G. M. Wolfe, K. T. Danas, J. B. Gilman, W. C. Kuster, D. M. Bon, A. Vlasenko, S.-M. Li, E. J. Williams, B. M. Lerner, P. R. Veres, J. M. Roberts, J. S. Holloway, B. Lefer, S. S. Brown, and J. A. Thornton
Atmos. Chem. Phys., 14, 3789–3800, https://doi.org/10.5194/acp-14-3789-2014, https://doi.org/10.5194/acp-14-3789-2014, 2014
F. D. Lopez-Hilfiker, C. Mohr, M. Ehn, F. Rubach, E. Kleist, J. Wildt, Th. F. Mentel, A. Lutz, M. Hallquist, D. Worsnop, and J. A. Thornton
Atmos. Meas. Tech., 7, 983–1001, https://doi.org/10.5194/amt-7-983-2014, https://doi.org/10.5194/amt-7-983-2014, 2014
S. E. Pusede, D. R. Gentner, P. J. Wooldridge, E. C. Browne, A. W. Rollins, K.-E. Min, A. R. Russell, J. Thomas, L. Zhang, W. H. Brune, S. B. Henry, J. P. DiGangi, F. N. Keutsch, S. A. Harrold, J. A. Thornton, M. R. Beaver, J. M. St. Clair, P. O. Wennberg, J. Sanders, X. Ren, T. C. VandenBoer, M. Z. Markovic, A. Guha, R. Weber, A. H. Goldstein, and R. C. Cohen
Atmos. Chem. Phys., 14, 3373–3395, https://doi.org/10.5194/acp-14-3373-2014, https://doi.org/10.5194/acp-14-3373-2014, 2014
R. L. N. Yatavelli, H. Stark, S. L. Thompson, J. R. Kimmel, M. J. Cubison, D. A. Day, P. Campuzano-Jost, B. B. Palm, A. Hodzic, J. A. Thornton, J. T. Jayne, D. R. Worsnop, and J. L. Jimenez
Atmos. Chem. Phys., 14, 1527–1546, https://doi.org/10.5194/acp-14-1527-2014, https://doi.org/10.5194/acp-14-1527-2014, 2014
B. Friedman, A. Zelenyuk, J. Beranek, G. Kulkarni, M. Pekour, A. Gannet Hallar, I. B. McCubbin, J. A. Thornton, and D. J Cziczo
Atmos. Chem. Phys., 13, 11839–11851, https://doi.org/10.5194/acp-13-11839-2013, https://doi.org/10.5194/acp-13-11839-2013, 2013
K. Ruusuvuori, T. Kurtén, I. K. Ortega, J. Faust, and H. Vehkamäki
Atmos. Chem. Phys., 13, 10397–10404, https://doi.org/10.5194/acp-13-10397-2013, https://doi.org/10.5194/acp-13-10397-2013, 2013
M. Paramonov, P. P. Aalto, A. Asmi, N. Prisle, V.-M. Kerminen, M. Kulmala, and T. Petäjä
Atmos. Chem. Phys., 13, 10285–10301, https://doi.org/10.5194/acp-13-10285-2013, https://doi.org/10.5194/acp-13-10285-2013, 2013
P. M. Edwards, C. J. Young, K. Aikin, J. deGouw, W. P. Dubé, F. Geiger, J. Gilman, D. Helmig, J. S. Holloway, J. Kercher, B. Lerner, R. Martin, R. McLaren, D. D. Parrish, J. Peischl, J. M. Roberts, T. B. Ryerson, J. Thornton, C. Warneke, E. J. Williams, and S. S. Brown
Atmos. Chem. Phys., 13, 8955–8971, https://doi.org/10.5194/acp-13-8955-2013, https://doi.org/10.5194/acp-13-8955-2013, 2013
N. Bork, T. Kurtén, and H. Vehkamäki
Atmos. Chem. Phys., 13, 3695–3703, https://doi.org/10.5194/acp-13-3695-2013, https://doi.org/10.5194/acp-13-3695-2013, 2013
N. L. Prisle, N. Ottosson, G. Öhrwall, J. Söderström, M. Dal Maso, and O. Björneholm
Atmos. Chem. Phys., 12, 12227–12242, https://doi.org/10.5194/acp-12-12227-2012, https://doi.org/10.5194/acp-12-12227-2012, 2012
J. S. Craven, L. D. Yee, N. L. Ng, M. R. Canagaratna, C. L. Loza, K. A. Schilling, R. L. N. Yatavelli, J. A. Thornton, P. J. Ziemann, R. C. Flagan, and J. H. Seinfeld
Atmos. Chem. Phys., 12, 11795–11817, https://doi.org/10.5194/acp-12-11795-2012, https://doi.org/10.5194/acp-12-11795-2012, 2012
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Source contribution to ozone pollution during June 2021 fire events in Arizona: insights from WRF-Chem-tagged O3 and CO
High-resolution mapping of on-road vehicle emissions with real-time traffic datasets based on big data
Sensitivity of climate–chemistry model simulated atmospheric composition to the application of an inverse relationship between NOx emission and lightning flash frequency
Regional and sectoral contributions of NOx and reactive carbon emission sources to global trends in tropospheric ozone during the 2000–2018 period
Underappreciated contributions of biogenic volatile organic compounds from urban green spaces to ozone pollution
Chemistry–climate feedback of atmospheric methane in a methane-emission-flux-driven chemistry–climate model
Surface ozone trend variability across the United States and the impact of heat waves (1990–2023)
Sensitivity of climate effects of hydrogen to leakage size, location, and chemical background
Evaluating tropospheric nitrogen dioxide in UKCA using OMI satellite retrievals over south and east Asia
Technical note: A comparative study of chemistry schemes for volcanic sulfur dioxide in Lagrangian transport simulations – a case study of the 2019 Raikoke eruption
Revisiting the high tropospheric ozone over southern Africa: role of biomass burning and anthropogenic emissions
Monoterpene oxidation pathways initiated by acyl peroxy radical addition
Local and transboundary contributions to NOy loadings across East Asia using CMAQ-ISAM and a GEMS-informed emission inventory during the winter–spring transition
Estimating the variability in NOx emissions from Wuhan with TROPOMI NO2 data during 2018 to 2023
Enhanced understanding of atmospheric blocking modulation on ozone dynamics within a high-resolution Earth system model
Natural emissions of VOC and NOx over Africa constrained by TROPOMI HCHO and NO2 data using the MAGRITTEv1.1 model
Contributions of lightning to long-term trends and inter-annual variability in global atmospheric chemistry constrained by Schumann Resonance observations
Impacts of wildfire smoke aerosols on near-surface ozone photochemistry
Anthropogenic emission controls reduce summertime ozone–temperature sensitivity in the United States
Investigating the response of China's surface ozone concentration to the future changes of multiple factors
Assessing the relative impacts of satellite ozone and its precursor observations to improve global tropospheric ozone analysis using multiple chemical reanalysis systems
Evaluating present-day and future impacts of agricultural ammonia emissions on atmospheric chemistry and climate
Air-pollution-satellite-based CO2 emission inversion: system evaluation, sensitivity analysis, and future research direction
Insights into ozone pollution control in urban areas by decoupling meteorological factors based on machine learning
Quantification of regional net CO2 flux errors in the Orbiting Carbon Observatory-2 (OCO-2) v10 model intercomparison project (MIP) ensemble using airborne measurements
Reactive nitrogen in and around the northeastern and mid-Atlantic US: sources, sinks, and connections with ozone
Preindustrial-to-present-day changes in atmospheric carbon monoxide: agreement and gaps between ice archives and global model reconstructions
Investigating processes influencing simulation of local Arctic wintertime anthropogenic pollution in Fairbanks, Alaska, during ALPACA-2022
Urban ozone formation and sensitivities to volatile chemical products, cooking emissions, and NOx upwind of and within two Los Angeles Basin cities
Causes of growing middle-to-upper tropospheric ozone over the northwest Pacific region
Impact of introducing electric vehicles on ground-level O3 and PM2.5 in the Greater Tokyo Area: yearly trends and the importance of changes in the urban heat island effect
Modelling Arctic Lower Tropospheric Ozone: processes controlling seasonal variations
Climate-driven biogenic emissions alleviate the impact of man-made emission reduction on O3 control in Pearl River Delta region, southern China
South Asia ammonia emission inversion through assimilating IASI observations
Constraining the budget of NOx and VOCs at a remote Tropical island using multi-platform observations and WRF-Chem model simulations
A CO2–Δ14CO2 inversion setup for estimating European fossil CO2 emissions
Maximum ozone concentrations in the southwestern US and Texas: implications of the growing predominance of the background contribution
Derivation of atmospheric reaction mechanisms for volatile organic compounds by the SAPRC mechanism generation system (MechGen)
Comparative ozone production sensitivity to NOx and VOCs in Quito, Ecuador and Santiago, Chile: implications for control strategies in times of climate action
Seasonal, regional, and vertical characteristics of high-carbon-monoxide plumes along with their associated ozone anomalies, as seen by IAGOS between 2002 and 2019
Tropospheric ozone trends and attributions over East and Southeast Asia in 1995–2019: An integrated assessment using statistical methods, machine learning models, and multiple chemical transport models
The potential of drone observations to improve air quality predictions by 4D-Var
Process analysis of elevated concentrations of organic acids at Whiteface Mountain, New York
Ozone source attribution in polluted European areas during summer 2017 as simulated with MECO(n)
Characterization of reactive nitrogen in the global upper troposphere using recent and historical commercial and research aircraft campaigns and GEOS-Chem
Opinion: Challenges and needs of tropospheric chemical mechanism development
Decrease of the European NOx anthropogenic emissions between 2005 and 2019 as seen from the OMI and TROPOMI NO2 satellite observations
Rapid Increases of Ozone Concentrations over Tibetan Plateau Caused by Local and Non-Local Factors
Tracking daily NOx emissions from an urban agglomeration based on TROPOMI NO2 and a local ensemble transform Kalman filter
The atmospheric oxidizing capacity in China – Part 2: Sensitivity to emissions of primary pollutants
Yafang Guo, Mohammad Amin Mirrezaei, Armin Sorooshian, and Avelino F. Arellano
Atmos. Chem. Phys., 25, 5591–5616, https://doi.org/10.5194/acp-25-5591-2025, https://doi.org/10.5194/acp-25-5591-2025, 2025
Short summary
Short summary
We assess the contributions of fire and anthropogenic emissions to O3 levels in Phoenix, Arizona, during a period of intense heat and drought conditions. We find that fire exacerbates O3 pollution and that interactions between weather, climate, and air chemistry are important to consider. This has implications for activities related to formulating emission reduction strategies in areas that are currently understudied yet becoming relevant due to reports of increasing global aridity.
Yujia Wang, Hongbin Wang, Bo Zhang, Peng Liu, Xinfeng Wang, Shuchun Si, Likun Xue, Qingzhu Zhang, and Qiao Wang
Atmos. Chem. Phys., 25, 5537–5555, https://doi.org/10.5194/acp-25-5537-2025, https://doi.org/10.5194/acp-25-5537-2025, 2025
Short summary
Short summary
This study established a bottom-up approach that employs real-time traffic flows and interpolation to obtain a spatially continuous on-road vehicle emission mapping for the main urban area of Jinan. The diurnal variation, spatial distribution, and emission hotspots were analyzed with clustering and hotspot analysis, showing unique fine-scale variation characteristics of on-road vehicle emissions. Future scenario analysis demonstrates remarkable benefits of electrification on emission reduction.
Francisco J. Pérez-Invernón, Francisco J. Gordillo-Vázquez, Heidi Huntrieser, Patrick Jöckel, and Eric J. Bucsela
Atmos. Chem. Phys., 25, 5557–5575, https://doi.org/10.5194/acp-25-5557-2025, https://doi.org/10.5194/acp-25-5557-2025, 2025
Short summary
Short summary
Lightning plays a significant role in tropospheric chemistry by producing substantial amounts of nitrogen oxides. According to recent estimates, thunderstorms that produce a higher lightning frequency rate also produce less nitrogen oxide per flash. We implemented the dependency of nitrogen oxide production per flash on lightning flash frequency in a chemical atmospheric model.
Aditya Nalam, Aura Lupaşcu, Tabish Ansari, and Tim Butler
Atmos. Chem. Phys., 25, 5287–5311, https://doi.org/10.5194/acp-25-5287-2025, https://doi.org/10.5194/acp-25-5287-2025, 2025
Short summary
Short summary
Tropospheric O3 molecules are labeled with the identity of their precursor source to simulate contributions from various emission sources to the global tropospheric O3 burden (TOB) and its trends. With an equatorward shift, anthropogenic NOx emissions become significantly more efficient at producing O3 and play a major role in driving TOB trends, mainly due to larger convection at the tropics effectively lifting O3 and its precursors to the free troposphere, where O3 lifetime is longer.
Haofan Wang, Yuejin Li, Yiming Liu, Xiao Lu, Yang Zhang, Qi Fan, Chong Shen, Senchao Lai, Yan Zhou, Tao Zhang, and Dingli Yue
Atmos. Chem. Phys., 25, 5233–5250, https://doi.org/10.5194/acp-25-5233-2025, https://doi.org/10.5194/acp-25-5233-2025, 2025
Short summary
Short summary
This study explores how urban green spaces (UGSs) in Guangzhou influence ozone levels. By using advanced models, we found that natural emissions from these areas can significantly affect air quality. Our results suggest that the design and planning of UGSs should not only consider aesthetics and social factors but also their environmental impacts on air quality.
Laura Stecher, Franziska Winterstein, Patrick Jöckel, Michael Ponater, Mariano Mertens, and Martin Dameris
Atmos. Chem. Phys., 25, 5133–5158, https://doi.org/10.5194/acp-25-5133-2025, https://doi.org/10.5194/acp-25-5133-2025, 2025
Short summary
Short summary
Methane, the second most important anthropogenic greenhouse gas, is chemically decomposed in the atmosphere. The chemical sink of atmospheric methane is not constant but depends on the temperature and on the abundance of its reaction partners. In this study, we use a global chemistry–climate model to assess the feedback of atmospheric methane induced by changes in the chemical sink in a warming climate and its implications for the chemical composition and the surface air temperature change.
Kai-Lan Chang, Brian C. McDonald, Colin Harkins, and Owen R. Cooper
Atmos. Chem. Phys., 25, 5101–5132, https://doi.org/10.5194/acp-25-5101-2025, https://doi.org/10.5194/acp-25-5101-2025, 2025
Short summary
Short summary
Exposure to high levels of ozone can be harmful to human health. This study shows consistent and robust evidence of decreasing ozone extremes across much of the United States over the period from 1990 to 2023, previously attributed to ozone precursor emission controls. Nevertheless, we also show that the increasing heat wave frequencies are likely to contribute to additional ozone exceedances, slowing the progress of decreasing the frequency of ozone exceedances.
Ragnhild Bieltvedt Skeie, Marit Sandstad, Srinath Krishnan, Gunnar Myhre, and Maria Sand
Atmos. Chem. Phys., 25, 4929–4942, https://doi.org/10.5194/acp-25-4929-2025, https://doi.org/10.5194/acp-25-4929-2025, 2025
Short summary
Short summary
Hydrogen leakages can alter the amount of climate gases in the atmosphere and hence have a climate impact. In this study we investigate, using an atmospheric chemistry model, how this indirect climate effect differs with different amounts of leakages and with where the hydrogen leaks and if this effect changes in the future. The effect is largest for emissions far from areas where hydrogen is removed from the atmosphere by the soil, but these are not relevant locations for a future hydrogen economy.
Alok K. Pandey, David S. Stevenson, Alcide Zhao, Richard J. Pope, Ryan Hossaini, Krishan Kumar, and Martyn P. Chipperfield
Atmos. Chem. Phys., 25, 4785–4802, https://doi.org/10.5194/acp-25-4785-2025, https://doi.org/10.5194/acp-25-4785-2025, 2025
Short summary
Short summary
Nitrogen dioxide is an air pollutant largely controlled by human activity that affects ozone, methane, and aerosols. Satellite instruments can quantify column NO2 and, by carefully matching the time and location of measurements, enable evaluation of model simulations. NO2 over south and east Asia is assessed, showing that the model captures not only many features of the measurements, but also important differences that suggest model deficiencies in representing several aspects of the atmospheric chemistry of NO2.
Mingzhao Liu, Lars Hoffmann, Jens-Uwe Grooß, Zhongyin Cai, Sabine Grießbach, and Yi Heng
Atmos. Chem. Phys., 25, 4403–4418, https://doi.org/10.5194/acp-25-4403-2025, https://doi.org/10.5194/acp-25-4403-2025, 2025
Short summary
Short summary
We studied the transport and chemical decomposition of volcanic SO2, focusing on the 2019 Raikoke event. By comparing two different chemistry modeling schemes, we found that including complex chemical reactions leads to a more accurate prediction of how long SO2 stays in the atmosphere. This research helps improve our understanding of volcanic pollution and its impact on air quality and climate, providing better tools for scientists to track and predict the movement of these pollutants.
Yufen Wang, Ke Li, Xi Chen, Zhenjiang Yang, Minglong Tang, Pascoal M. D. Campos, Yang Yang, Xu Yue, and Hong Liao
Atmos. Chem. Phys., 25, 4455–4475, https://doi.org/10.5194/acp-25-4455-2025, https://doi.org/10.5194/acp-25-4455-2025, 2025
Short summary
Short summary
The impacts of biomass burning and anthropogenic emissions on high tropospheric ozone levels are not well studied in southern Africa. We combined model simulations with recent observations at the surface and from space to quantify tropospheric ozone and its drivers in southern Africa. Our work focuses on the impact of emissions from different sources at different spatial scales, contributing to a comprehensive understanding of air pollution drivers and their uncertainties in southern Africa.
Dominika Pasik, Thomas Golin Almeida, Emelda Ahongshangbam, Siddharth Iyer, and Nanna Myllys
Atmos. Chem. Phys., 25, 4313–4331, https://doi.org/10.5194/acp-25-4313-2025, https://doi.org/10.5194/acp-25-4313-2025, 2025
Short summary
Short summary
We used quantum chemistry methods to investigate the oxidation mechanisms of acyl peroxy radicals (APRs) with various monoterpenes. Our findings reveal unique oxidation pathways for different monoterpenes, leading to either chain-terminating products or highly reactive intermediates that can contribute to particle formation in the atmosphere. This research highlights APRs as potentially significant but underexplored atmospheric oxidants that may influence future approaches to modelling climate.
Jincheol Park, Yunsoo Choi, and Sagun Kayastha
Atmos. Chem. Phys., 25, 4291–4311, https://doi.org/10.5194/acp-25-4291-2025, https://doi.org/10.5194/acp-25-4291-2025, 2025
Short summary
Short summary
We investigated NOx emission contributions to NOy loadings across five regions of East Asia during the 2022 winter–spring transition through chemical transport modeling informed by satellite data. As seasons progress, local contributions within each region to its NOy budget decreased from 32 %–43 % to 23 %–30 %, while transboundary contributions increased from 16 %–33 % to 27 %–37 %, driven by a shift in synoptic settings that allowed pollutants to spread more broadly across the regions.
Qianqian Zhang, K. Folkert Boersma, Chiel van der Laan, Alba Mols, Bin Zhao, Shengyue Li, and Yuepeng Pan
Atmos. Chem. Phys., 25, 3313–3326, https://doi.org/10.5194/acp-25-3313-2025, https://doi.org/10.5194/acp-25-3313-2025, 2025
Short summary
Short summary
Accurate NOx emission estimates are required to better understand air pollution. This study investigates and demonstrates the ability of the superposition column model in combination with TROPOMI tropospheric NO2 column data to estimate city-scale NOx emissions and lifetimes and their variabilities. The results of this work nevertheless confirm the strength of the superposition column model in estimating urban NOx emissions with reasonable accuracy.
Wenbin Kou, Yang Gao, Dan Tong, Xiaojie Guo, Xiadong An, Wenyu Liu, Mengshi Cui, Xiuwen Guo, Shaoqing Zhang, Huiwang Gao, and Lixin Wu
Atmos. Chem. Phys., 25, 3029–3048, https://doi.org/10.5194/acp-25-3029-2025, https://doi.org/10.5194/acp-25-3029-2025, 2025
Short summary
Short summary
Unlike traditional numerical studies, we apply a high-resolution Earth system model, improving simulations of surface ozone and large-scale circulations such as atmospheric blocking. Besides local heat waves, we quantify the impact of atmospheric blocking on downstream ozone concentrations, which is closely associated with the blocking position. We identify three major pathways of Rossby wave propagation, stressing the critical role of large-scale circulation in regional air quality.
Beata Opacka, Trissevgeni Stavrakou, Jean-François Müller, Isabelle De Smedt, Jos van Geffen, Eloise A. Marais, Rebekah P. Horner, Dylan B. Millet, Kelly C. Wells, and Alex B. Guenther
Atmos. Chem. Phys., 25, 2863–2894, https://doi.org/10.5194/acp-25-2863-2025, https://doi.org/10.5194/acp-25-2863-2025, 2025
Short summary
Short summary
Vegetation releases biogenic volatile organic compounds, while soils and lightning contribute to the natural emissions of nitrogen oxides into the atmosphere. These gases interact in complex ways. Using satellite data and models, we developed a new method to simultaneously optimize these natural emissions over Africa in 2019. Our approach resulted in an increase in natural emissions, supported by independent data indicating that current estimates are underestimated.
Xiaobo Wang, Yuzhong Zhang, Tamás Bozóki, Ruosi Liang, Xinchun Xie, Shutao Zhao, Rui Wang, Yujia Zhao, and Shuai Sun
EGUsphere, https://doi.org/10.5194/egusphere-2025-370, https://doi.org/10.5194/egusphere-2025-370, 2025
Short summary
Short summary
Schumann Resonance observations are used to parameterize lightning NOx emissions for better capturing global lightning trend and variability. Updated simulations reveal insignificant trend but greater variability in lightning NOx emissions, impacting tropospheric NOx, O3 and OH. Lightning generally counteracts non-lightning factors, reducing the inter-annua variability of tropospheric O3 and OH. Variations of global lightning play important role in understanding the atmospheric methane budget.
Jiaqi Shen, Ronald C. Cohen, Glenn M. Wolfe, and Xiaomeng Jin
EGUsphere, https://doi.org/10.5194/egusphere-2025-706, https://doi.org/10.5194/egusphere-2025-706, 2025
Short summary
Short summary
This study shows large chemical and radiative effects of smoke aerosols from fires on near-surface ozone production. Aerosol loading and NOx levels are identified as the primary factors influencing these effects. Furthermore, we show that the surface PM2.5 to NO2 column ratio can be used as an indicator for identifying aerosol-dominated regimes, facilitating the assessments of aerosol impacts on ozone formation through satellite observations.
Shuai Li, Haolin Wang, and Xiao Lu
Atmos. Chem. Phys., 25, 2725–2743, https://doi.org/10.5194/acp-25-2725-2025, https://doi.org/10.5194/acp-25-2725-2025, 2025
Short summary
Short summary
Summertime ozone–temperature sensitivity has decreased by 50 % from 3.0 ppbv per K in 1990 to 1.5 ppb per K in 2021 in the US. GEOS-Chem simulations show that anthropogenic nitrogen oxide emission reduction is the dominant driver of ozone–temperature sensitivity decline by influencing both temperature direct and temperature indirect processes. Reduced ozone–temperature sensitivity has decreased ozone enhancement from low to high temperatures by an average of 6.8 ppbv across the US.
Jinya Yang, Yutong Wang, Lei Zhang, and Yu Zhao
Atmos. Chem. Phys., 25, 2649–2666, https://doi.org/10.5194/acp-25-2649-2025, https://doi.org/10.5194/acp-25-2649-2025, 2025
Short summary
Short summary
We develop a modeling framework to predict future ozone concentrations (till the 2060s) in China following an IPCC scenario. We evaluate the contributions of climatic, anthropogenic, and biogenic factors by season and region. We find persistent emission controls will alter the nonlinear response of ozone to its precursors and dominate the declining ozone level. The outcomes highlight the importance of human actions, even with a climate penalty on air quality.
Takashi Sekiya, Emanuele Emili, Kazuyuki Miyazaki, Antje Inness, Zhen Qu, R. Bradley Pierce, Dylan Jones, Helen Worden, William Y. Y. Cheng, Vincent Huijnen, and Gerbrand Koren
Atmos. Chem. Phys., 25, 2243–2268, https://doi.org/10.5194/acp-25-2243-2025, https://doi.org/10.5194/acp-25-2243-2025, 2025
Short summary
Short summary
Five global chemical reanalysis datasets were used to assess the relative impacts of assimilating satellite ozone and its precursor measurements on tropospheric ozone analyses for 2010. The multiple reanalysis system comparison allows an evaluation of the dependency of the impacts on different reanalysis systems. The results suggested the importance of satellite ozone and its precursor measurements for improving ozone analysis in the whole troposphere, with varying magnitudes among the systems.
Maureen Beaudor, Didier Hauglustaine, Juliette Lathière, Martin Van Damme, Lieven Clarisse, and Nicolas Vuichard
Atmos. Chem. Phys., 25, 2017–2046, https://doi.org/10.5194/acp-25-2017-2025, https://doi.org/10.5194/acp-25-2017-2025, 2025
Short summary
Short summary
Agriculture is the biggest ammonia (NH3) source, impacting air quality, climate, and ecosystems. Because of food demand, NH3 emissions are projected to rise by 2100. Using a global model, we analyzed the impact of present and future NH3 emissions generated from a land model. Our results show improved ammonia patterns compared to a reference inventory. Future scenarios predict up to 70 % increase in global NH3 burden, with significant changes in radiative forcing that can greatly elevate N2O.
Hui Li, Jiaxin Qiu, and Bo Zheng
Atmos. Chem. Phys., 25, 1949–1963, https://doi.org/10.5194/acp-25-1949-2025, https://doi.org/10.5194/acp-25-1949-2025, 2025
Short summary
Short summary
We conduct a sensitivity analysis with 31 tests on various factors including prior emissions, model resolution, satellite constraint, and other system configurations to assess the vulnerability of emission estimates across temporal, sectoral, and regional dimensions. This reveals the robustness of emissions estimated by this air-pollution-satellite-based CO2 emission inversion system, with relative change between tests and base inversion below 4.0 % for national annual NOx and CO2 emissions.
Yuqing Qiu, Xin Li, Wenxuan Chai, Yi Liu, Mengdi Song, Xudong Tian, Qiaoli Zou, Wenjun Lou, Wangyao Zhang, Juan Li, and Yuanhang Zhang
Atmos. Chem. Phys., 25, 1749–1763, https://doi.org/10.5194/acp-25-1749-2025, https://doi.org/10.5194/acp-25-1749-2025, 2025
Short summary
Short summary
The chemical reactions of ozone (O3) formation are related to meteorology and local emissions. Here, a random forest approach was used to eliminate the effects of meteorological factors (dispersion or transport) on O3 and its precursors. Variations in the sensitivity of O3 formation and the apportionment of emission sources were revealed after meteorological normalization. Our results suggest that meteorological variations should be considered when diagnosing O3 formation.
Jeongmin Yun, Junjie Liu, Brendan Byrne, Brad Weir, Lesley E. Ott, Kathryn McKain, Bianca C. Baier, Luciana V. Gatti, and Sebastien C. Biraud
Atmos. Chem. Phys., 25, 1725–1748, https://doi.org/10.5194/acp-25-1725-2025, https://doi.org/10.5194/acp-25-1725-2025, 2025
Short summary
Short summary
This study quantifies errors in regional net surface–atmosphere CO2 flux estimates from an inverse model ensemble using airborne CO2 measurements. Our results show that flux error estimates based on observations significantly exceed those computed from the ensemble spread of flux estimates in regions with high fossil fuel emissions. This finding suggests the presence of systematic biases in the inversion estimates, associated with errors in the fossil fuel emissions common to all models.
Min Huang, Gregory R. Carmichael, Kevin W. Bowman, Isabelle De Smedt, Andreas Colliander, Michael H. Cosh, Sujay V. Kumar, Alex B. Guenther, Scott J. Janz, Ryan M. Stauffer, Anne M. Thompson, Niko M. Fedkin, Robert J. Swap, John D. Bolten, and Alicia T. Joseph
Atmos. Chem. Phys., 25, 1449–1476, https://doi.org/10.5194/acp-25-1449-2025, https://doi.org/10.5194/acp-25-1449-2025, 2025
Short summary
Short summary
We use model simulations along with multiplatform, multidisciplinary observations and a range of analysis methods to estimate and understand the distributions, temporal changes, and impacts of reactive nitrogen and ozone over the most populous US region that has undergone significant environmental changes. Deposition, biogenic emissions, and extra-regional sources have been playing increasingly important roles in controlling pollutant budgets in this area as local anthropogenic emissions drop.
Xavier Faïn, Sophie Szopa, Vaishali Naïk, Patricia Martinerie, David M. Etheridge, Rachael H. Rhodes, Cathy M. Trudinger, Vasilii V. Petrenko, Kévin Fourteau, and Philip Place
Atmos. Chem. Phys., 25, 1105–1119, https://doi.org/10.5194/acp-25-1105-2025, https://doi.org/10.5194/acp-25-1105-2025, 2025
Short summary
Short summary
Carbon monoxide (CO) plays a crucial role in the atmosphere's oxidizing capacity. In this study, we analyse how historical (1850–2014) [CO] outputs from state-of-the-art global chemistry–climate models over Greenland and Antarctica are able to capture both absolute values and trends recorded in multi-site ice archives. A disparity in [CO] growth rates emerges in the Northern Hemisphere between models and observations from 1920–1975 CE, possibly linked to uncertainties in CO emission factors.
Natalie Brett, Kathy S. Law, Steve R. Arnold, Javier G. Fochesatto, Jean-Christophe Raut, Tatsuo Onishi, Robert Gilliam, Kathleen Fahey, Deanna Huff, George Pouliot, Brice Barret, Elsa Dieudonné, Roman Pohorsky, Julia Schmale, Andrea Baccarini, Slimane Bekki, Gianluca Pappaccogli, Federico Scoto, Stefano Decesari, Antonio Donateo, Meeta Cesler-Maloney, William Simpson, Patrice Medina, Barbara D'Anna, Brice Temime-Roussel, Joel Savarino, Sarah Albertin, Jingqiu Mao, Becky Alexander, Allison Moon, Peter F. DeCarlo, Vanessa Selimovic, Robert Yokelson, and Ellis S. Robinson
Atmos. Chem. Phys., 25, 1063–1104, https://doi.org/10.5194/acp-25-1063-2025, https://doi.org/10.5194/acp-25-1063-2025, 2025
Short summary
Short summary
Processes influencing dispersion of local anthropogenic pollution in Arctic wintertime are investigated with Lagrangian dispersion modelling. Simulated power plant plume rise that considers temperature inversion layers improves results compared to observations (interior Alaska). Modelled surface concentrations are improved by representation of vertical mixing and emission estimates. Large increases in diesel vehicle emissions at temperatures reaching −35°C are required to reproduce observed NOx.
Chelsea E. Stockwell, Matthew M. Coggon, Rebecca H. Schwantes, Colin Harkins, Bert Verreyken, Congmeng Lyu, Qindan Zhu, Lu Xu, Jessica B. Gilman, Aaron Lamplugh, Jeff Peischl, Michael A. Robinson, Patrick R. Veres, Meng Li, Andrew W. Rollins, Kristen Zuraski, Sunil Baidar, Shang Liu, Toshihiro Kuwayama, Steven S. Brown, Brian C. McDonald, and Carsten Warneke
Atmos. Chem. Phys., 25, 1121–1143, https://doi.org/10.5194/acp-25-1121-2025, https://doi.org/10.5194/acp-25-1121-2025, 2025
Short summary
Short summary
In urban areas, emissions from everyday products like paints, cleaners, and personal care products, along with non-traditional sources such as cooking, are increasingly important and impact air quality. This study uses a box model to evaluate how these emissions impact ozone in the Los Angeles Basin and quantifies the impact of gaseous cooking emissions. Accurate representation of these and other anthropogenic sources in inventories is crucial for informing effective air quality policies.
Xiaodan Ma, Jianping Huang, Michaela I. Hegglin, Patrick Jöckel, and Tianliang Zhao
Atmos. Chem. Phys., 25, 943–958, https://doi.org/10.5194/acp-25-943-2025, https://doi.org/10.5194/acp-25-943-2025, 2025
Short summary
Short summary
Our research explored changes in ozone levels in the northwest Pacific region over 30 years, revealing a significant increase in the middle-to-upper troposphere, especially during spring and summer. This rise is influenced by both stratospheric and tropospheric sources, which affect climate and air quality in East Asia. This work underscores the need for continued study to understand underlying mechanisms.
Hiroo Hata, Norifumi Mizushima, and Tomohiko Ihara
Atmos. Chem. Phys., 25, 1037–1061, https://doi.org/10.5194/acp-25-1037-2025, https://doi.org/10.5194/acp-25-1037-2025, 2025
Short summary
Short summary
The introduction of battery electric vehicles (BEVs) is expected to reduce the primary air pollutants from vehicular exhaust and evaporative emissions while reducing the anthropogenic heat produced by vehicles, ultimately mitigating the urban heat island (UHI) effect. This study revealed the impact of introducing BEVs on the decrease in the UHI effect and the impact of BEVs on the formation of tropospheric ozone and fine particulate matter in the Greater Tokyo Area of Japan.
Wanmin Gong, Stephen R. Beagley, Kenjiro Toyota, Henrik Skov, Jesper Heile Christensen, Alexandru Lupu, Diane Pendlebury, Junhua Zhang, Ulas Im, Yugo Kanaya, Alfonso Saiz-Lopez, Roberto Sommariva, Peter Effertz, John W. Halfacre, Nis Jepsen, Rigel Kivi, Theodore K. Koenig, Katrin Müller, Claus Nordstrøm, Irina Petropavlovskikh, Paul B. Shepson, William R. Simpson, Sverre Solberg, Ralf M. Staebler, David W. Tarasick, Roeland Van Malderen, and Mika Vestenius
EGUsphere, https://doi.org/10.5194/egusphere-2024-3750, https://doi.org/10.5194/egusphere-2024-3750, 2025
Short summary
Short summary
This study showed that the springtime O3 depletion plays a critical role in driving the surface O3 seasonal cycle in Central Arctic. The O3 depletion events, while occurring most notably within the lowest few hundred metres above the Arctic Ocean, can induce a 5–7 % of loss in the pan-Arctic tropospheric O3 burden during springtime. The study also found an enhancement in O3 and NOy (mostly PAN) concentrations in the Arctic due to northern boreal wildfires, particularly at altitudes.
Nan Wang, Song Liu, Jiawei Xu, Yanyu Wang, Chun Li, Hua Lu, and Fumo Yang
EGUsphere, https://doi.org/10.5194/egusphere-2024-3771, https://doi.org/10.5194/egusphere-2024-3771, 2025
Short summary
Short summary
We found that climate warming and changes in vegetation have increased biogenic volatile organic compound emissions in the Pearl River Delta region. These increasing natural emissions, mainly due to climate warming, are weakening the benefits of reducing man-made emission control, leading to higher ozone levels. This work helps us understand how climate change influences air quality and provides important insights for improving pollution control strategies in the future.
Ji Xia, Yi Zhou, Li Fang, Yingfei Qi, Dehao Li, Hong Liao, and Jianbing Jin
EGUsphere, https://doi.org/10.5194/egusphere-2024-3938, https://doi.org/10.5194/egusphere-2024-3938, 2025
Short summary
Short summary
This study established an ammonia emission inventory in South Asia via assimilation-based inversion system. The posterior emissions, calculated by integrating the CEDS inventory and IASI satellite observations, showed significant improvement over the prior. Validation against various measurements all support our posterior emission. It offers valuable insights of ammonia emissions for policymakers and researchers aiming to develop air quality management and mitigation strategies there.
Catalina Poraicu, Jean-François Müller, Trissevgeni Stavrakou, Crist Amelynck, Bert W. D. Verreyken, Niels Schoon, Corinne Vigouroux, Nicolas Kumps, Jérôme Brioude, Pierre Tulet, and Camille Mouchel-Vallon
EGUsphere, https://doi.org/10.5194/egusphere-2024-3555, https://doi.org/10.5194/egusphere-2024-3555, 2025
Short summary
Short summary
We investigated the sources and impacts of nitrogen oxides and organic compounds over a remote tropical island. High-resolution WRF-Chem simulations were evaluated using in situ, FTIR and satellite measurements. This work highlights gaps in current models, like missing sources of key organic compounds and inaccuracies in emission inventories, emphasizing the importance of improving chemical and dynamical processes in atmospheric modelling for budget estimates in tropical regions.
Carlos Gómez-Ortiz, Guillaume Monteil, Sourish Basu, and Marko Scholze
Atmos. Chem. Phys., 25, 397–424, https://doi.org/10.5194/acp-25-397-2025, https://doi.org/10.5194/acp-25-397-2025, 2025
Short summary
Short summary
In this paper, we test new implementations of our inverse modeling tool to estimate the weekly and regional CO2 emissions from fossil fuels in Europe. We use synthetic atmospheric observations of CO2 and radiocarbon (14CO2) to trace emissions to their sources, while separating the natural and fossil CO2. Our tool accurately estimates fossil CO2 emissions in densely monitored regions like western/central Europe. This approach aids in developing strategies for reducing CO2 emissions.
David D. Parrish, Ian C. Faloona, and Richard G. Derwent
Atmos. Chem. Phys., 25, 263–289, https://doi.org/10.5194/acp-25-263-2025, https://doi.org/10.5194/acp-25-263-2025, 2025
Short summary
Short summary
Observation-based estimates of contributions to maximum ozone (O3) concentrations show that background O3 can exceed the air quality standard of 70 ppb in the southwestern US, precluding standard attainment. Over the past 4 decades, US anthropogenic O3 has decreased by a factor of ~ 6.3, while wildfire contributions have increased, so that the background now dominates maximum concentrations, even in Los Angeles, and the occurrence of maximum O3 has shifted from the eastern to the western US.
William P. L. Carter, Jia Jiang, John J. Orlando, and Kelley C. Barsanti
Atmos. Chem. Phys., 25, 199–242, https://doi.org/10.5194/acp-25-199-2025, https://doi.org/10.5194/acp-25-199-2025, 2025
Short summary
Short summary
This paper describes the scientific basis for gas-phase atmospheric chemical mechanisms derived using the SAPRC mechanism generation system, MechGen. It can derive mechanisms for most organic compounds with C, H, O, or N atoms, including initial reactions of organics with OH, O3, NO3, and O3P or by photolysis, as well as the reactions of the various types of intermediates that are formed. The paper includes a description of areas of uncertainty where additional research and updates are needed.
María Cazorla, Melissa Trujillo, Rodrigo Seguel, and Laura Gallardo
EGUsphere, https://doi.org/10.5194/egusphere-2024-3720, https://doi.org/10.5194/egusphere-2024-3720, 2024
Short summary
Short summary
The current climate emergency imposes the need to take actions in cities to curb ozone as a pollutant and a climate forcer. In this work we analyze how reducing the levels of ozone precursor would affect photochemical smog in Quito, Ecuador and Santiago, Chile. Results show that if environmental policy were implemented to reduce only nitrogen oxides, the production of ozone would increase substantially for which more integral solutions are needed.
Thibaut Lebourgeois, Bastien Sauvage, Pawel Wolff, Béatrice Josse, Virginie Marécal, Yasmine Bennouna, Romain Blot, Damien Boulanger, Hannah Clark, Jean-Marc Cousin, Philippe Nedelec, and Valérie Thouret
Atmos. Chem. Phys., 24, 13975–14004, https://doi.org/10.5194/acp-24-13975-2024, https://doi.org/10.5194/acp-24-13975-2024, 2024
Short summary
Short summary
Our study examines intense-carbon-monoxide (CO) pollution events measured by commercial aircraft from the In-service Aircraft for a Global Observing System (IAGOS) research infrastructure. We combine these measurements with the SOFT-IO model to trace the origin of the observed CO. A comprehensive analysis of the geographical origin, source type, seasonal variation, and ozone levels of these pollution events is provided.
Xiao Lu, Yiming Liu, Jiayin Su, Xiang Weng, Tabish Ansari, Yuqiang Zhang, Guowen He, Yuqi Zhu, Haolin Wang, Ganquan Zeng, Jingyu Li, Cheng He, Shuai Li, Teerachai Amnuaylojaroen, Tim Butler, Qi Fan, Shaojia Fan, Grant L. Forster, Meng Gao, Jianlin Hu, Yugo Kanaya, Mohd Talib Latif, Keding Lu, Philippe Nédélec, Peer Nowack, Bastien Sauvage, Xiaobin Xu, Lin Zhang, Ke Li, Ja-Ho Koo, and Tatsuya Nagashima
EGUsphere, https://doi.org/10.5194/egusphere-2024-3702, https://doi.org/10.5194/egusphere-2024-3702, 2024
Short summary
Short summary
This study analyzes summertime ozone trends in East and Southeast Asia derived from a comprehensive observational database spanning from 1995 to 2019, incorporating aircraft observations, ozonesonde data, and measurements from 2500 surface sites. Multiple models are applied to attribute to changes in anthropogenic emissions and climate. The results highlight increases in anthropogenic emission are the primary driver of ozone increases both in the free troposphere and at the surface.
Hassnae Erraji, Philipp Franke, Astrid Lampert, Tobias Schuldt, Ralf Tillmann, Andreas Wahner, and Anne Caroline Lange
Atmos. Chem. Phys., 24, 13913–13934, https://doi.org/10.5194/acp-24-13913-2024, https://doi.org/10.5194/acp-24-13913-2024, 2024
Short summary
Short summary
Four-dimensional variational data assimilation allows for the simultaneous optimisation of initial values and emission rates by using trace-gas profiles from drone observations in a regional air quality model. Assimilated profiles positively impact the representation of air pollutants in the model by improving their vertical distribution and ground-level concentrations. This case study highlights the potential of drone data to enhance air quality analyses including local emission evaluation.
Christopher Lawrence, Mary Barth, John Orlando, Paul Casson, Richard Brandt, Daniel Kelting, Elizabeth Yerger, and Sara Lance
Atmos. Chem. Phys., 24, 13693–13713, https://doi.org/10.5194/acp-24-13693-2024, https://doi.org/10.5194/acp-24-13693-2024, 2024
Short summary
Short summary
This work uses chemical transport and box modeling to study the gas- and aqueous-phase production of organic acid concentrations measured in cloud water at the summit of Whiteface Mountain on 1 July 2018. Isoprene was the major source of formic, acetic, and oxalic acid. Gas-phase chemistry greatly underestimated formic and acetic acid, indicating missing sources, while cloud chemistry was a key source of oxalic acid. More studies of organic acids are required to better constrain their sources.
Markus Kilian, Volker Grewe, Patrick Jöckel, Astrid Kerkweg, Mariano Mertens, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 24, 13503–13523, https://doi.org/10.5194/acp-24-13503-2024, https://doi.org/10.5194/acp-24-13503-2024, 2024
Short summary
Short summary
Anthropogenic emissions are a major source of precursors of tropospheric ozone. As ozone formation is highly non-linear, we apply a global–regional chemistry–climate model with a source attribution method (tagging) to quantify the contribution of anthropogenic emissions to ozone. Our analysis shows that the contribution of European anthropogenic emissions largely increases during large ozone periods, indicating that emissions from these sectors drive ozone values.
Nana Wei, Eloise A. Marais, Gongda Lu, Robert G. Ryan, and Bastien Sauvage
EGUsphere, https://doi.org/10.5194/egusphere-2024-3388, https://doi.org/10.5194/egusphere-2024-3388, 2024
Short summary
Short summary
This study uses reactive nitrogen observations from NASA DC-8 research aircraft and The In-service Aircraft for a Global Observing System (IAGOS) campaigns to characterise reactive nitrogen seasonality and composition in the global upper troposphere and to diagnose the greatest knowledge gaps from comparison to a state-of-science model GEOS-Chem that need to be resolved for climate, nitrogen cycle and air pollution assessments.
Barbara Ervens, Andrew Rickard, Bernard Aumont, William P. L. Carter, Max McGillen, Abdelwahid Mellouki, John Orlando, Bénédicte Picquet-Varrault, Paul Seakins, William R. Stockwell, Luc Vereecken, and Timothy J. Wallington
Atmos. Chem. Phys., 24, 13317–13339, https://doi.org/10.5194/acp-24-13317-2024, https://doi.org/10.5194/acp-24-13317-2024, 2024
Short summary
Short summary
Chemical mechanisms describe the chemical processes in atmospheric models that are used to describe the changes in the atmospheric composition. Therefore, accurate chemical mechanisms are necessary to predict the evolution of air pollution and climate change. The article describes all steps that are needed to build chemical mechanisms and discusses the advances and needs of experimental and theoretical research activities needed to build reliable chemical mechanisms.
Audrey Fortems-Cheiney, Grégoire Broquet, Robin Plauchu, Elise Potier, Antoine Berchet, Isabelle Pison, Adrien Martinez, Rimal Abeed, Gaelle Dufour, Adriana Coman, Dilek Savas, Guillaume Siour, Henk Eskes, Hugo A. C. Denier van der Gon, and Stijn N. C. Dellaert
EGUsphere, https://doi.org/10.5194/egusphere-2024-3679, https://doi.org/10.5194/egusphere-2024-3679, 2024
Short summary
Short summary
This study assesses the potential of the OMI and TROPOMI satellite observations to inform about the evolution of NOx anthropogenic emissions between year 2005 and year 2019 at the regional to national scales in Europe. Both the OMI and TROPOMI inversions show decreases in European NOx anthropogenic emission budgets between 2005 and 2019, but with different magnitudes.
Chenghao Xu, Jintai Lin, Hao Kong, Junli Jin, Lulu Chen, and Xiaobin Xu
EGUsphere, https://doi.org/10.5194/egusphere-2024-3471, https://doi.org/10.5194/egusphere-2024-3471, 2024
Short summary
Short summary
We observed a strong increase in deseasonalized ozone at urban stations on the Tibetan Plateau from 2015 to 2019, far exceeding the trend at the baseline station Waliguan and the Tibet Plateau average trend of four tropospheric ozone products. By combining multiple datasets and modeling approaches, we identified the main contributing factors as more frequent transport passing through the lower layers of high-emission regions and the rapid increase in anthropogenic nitrogen oxide emissions.
Yawen Kong, Bo Zheng, and Yuxi Liu
EGUsphere, https://doi.org/10.5194/egusphere-2024-2996, https://doi.org/10.5194/egusphere-2024-2996, 2024
Short summary
Short summary
Current high-resolution satellite remote sensing technologies provide a unique opportunity to derive timely, high-resolution emission data. We developed an emission inversion system to assimilate satellite NO2 data to obtain daily, kilometer-scale NOx emission inventories. Our results enhance inventory accuracy, allowing us to capture the effects of pollution control policies on daily emissions (e.g., during COVID-19 lockdown) and improve fine-scale air quality modeling.
Jianing Dai, Guy P. Brasseur, Mihalis Vrekoussis, Maria Kanakidou, Kun Qu, Yijuan Zhang, Hongliang Zhang, and Tao Wang
Atmos. Chem. Phys., 24, 12943–12962, https://doi.org/10.5194/acp-24-12943-2024, https://doi.org/10.5194/acp-24-12943-2024, 2024
Short summary
Short summary
This paper employs a regional chemical transport model to quantify the sensitivity of air pollutants and photochemical parameters to specified emission reductions in China for representative winter and summer conditions. The study provides insights into further air quality control in China with reduced primary emissions.
Cited articles
Adler, T. B., Knizia, G., and Werner, H. J.: A simple and efficient
CCSD(T)-F12 approximation, J. Chem. Phys., 127, 221106,
https://doi.org/10.1063/1.2817618, 2007.
Becke, A. D.: Density-functional exchange-energy approximation with correct
asymptotic behavior, Phys. Rev. A, 38, 3098–3100, 1988.
Bianchi, F., Kurtén, T., Riva, M., Mohr, C.,, Rissanen, M., Roldin, P.;
Berndt, T., Crounse, J., Wennberg, P., Mentel, T., Wildt, J., Junninen, H.,
Jokinen, T., Kulmala, M., Worsnop, D., Thornton, J., Donahue, N. M.,
Kjaergaard, H. G., and Ehn, M.: Highly oxygenated molecules (HOM) from gas-phase
autoxidation of organic peroxy radicals: A key contributor to atmospheric
aerosol. Chem. Rev., in review, 2018.
Bilde, M., Barsanti, K., Booth, M., Cappa, C. D., Donahue, N. M.,
Emanuelsson, E. U., McFiggans, G., Krieger, U. K., Marcolli, C., Topping,
D., Ziemann, P., Barley, M., Clegg, S., Dennis-Smither, B., Hallquist, M.,
Hallquist, Å. M., Khlystov, A., Kulmala, M., Mogensen, D.,
Percival, C. J., Pope, F., Reid, J. P., Ribeiro da Silva, M. A. V.,
Rosenörn, T., Salo, K., Soonsin, V. P., Yli-Juuti, T., Prisle, N. L.,
Pagels, J., Rarey, J., Zardini, A. A., and Riipinen, I.: Saturation Vapor
Pressures and Transition Enthalpies of Low-Volatility Organic Molecules of
Atmospheric Relevance: From Dicarboxylic Acids to Complex Mixtures, Chem.
Rev., 115, 4115–4156, https://doi.org/10.1021/cr5005502, 2015.
Brauer, M., Freedman, G., Frostad, J., van Donkelaar, A., Martin, R. V.,
Dentener, F., van Dingenen, R., Estep, K., Amini, H., Apte, J. S.,
Balakrishnan, K., Barregard, L., Broday, D., Feigin, V., Ghosh, S., Hopke,
P. K., Knibbs, L. D., Kokubo, Y., Liu, Y., Ma, S., Morawska, L., Texcalac
Sangrador, J. L., Shaddick, G., Anderson, R., Forouzanfar, M. H., Burnett,
R. T., and Cohen A.: Ambient Air Pollution Exposure Estimation for the Global
Burden of Disease 2013, Environ. Sci. Tech. Lett., 50, 79–88, 2016.
Chen, X., Oja, V., Chan, W. G., and Hajaligol, M. R.: Vapor Pressure
Characterization of Several Phenolics and Polyhydric Compounds by Knudsen
Effusion Method, J.Chem. Eng. Data, 51, 386–391,
2006.
Compernolle, S., Ceulemans, K., and Müller, J.-F.: EVAPORATION: a new vapour
pressure estimation methodfor organic molecules including non-additivity and
intramolecular interactions, Atmos. Chem. Phys., 11, 9431–9450,
https://doi.org/10.5194/acp-11-9431-2011, 2011.
COSMOconf: Version 4.2, COSMOlogic GmbH & Co KG, available at:
http://www.cosmologic.de, last access: 7 May 2018, 2017.
COSMOtherm: version C3.0, Release 18.00, COSMOlogic GmbH & Co. KG,
available at: http://www.cosmologic.de, last access: 7 May 2018.
D'Ambro, E. L., Lee, B. H., Liu, J., Shilling, J. E., Gaston, C. J.,
Lopez-Hilfiker, F. D., Schobesberger, S., Zaveri, R. A., Mohr, C., Lutz, A.,
Zhang, Z., Gold, A., Surratt, J. D., Rivera-Rios, J. C., Keutsch, F. N., and
Thornton, J. A.: Molecular composition and volatility of isoprene
photochemical oxidation secondary organic aerosol under low- and
high-NOx
conditions, Atmos. Chem. Phys., 17, 159–174,
https://doi.org/10.5194/acp-17-159-2017, 2017.
Eckert, F. and Klamt, A.: Fast solvent screening via quantum chemistry:
COSMO-RS approach, AlChE J., 48, 369–385, 2002.
Ehn, M., Thornton, J. A., Kleist, E., Sipila, M., Junninen, H., Pullinen,
I., Springer, M., Rubach, F., Tillmann, R., Lee, B., Lopez-Hilfiker, F.,
Andres, S., Acir, I.-H., Rissanen, M., Jokinen, T., Schobesberger, S.,
Kangasluoma, J., Kontkanen, J., Nieminen, T., Kurten, T., Nielsen, L. B.,
Jorgensen, S., Kjaergaard, H. G., Canagaratna, M., Maso, M. D., Berndt, T.,
Petaja, T., Wahner, A., Kerminen, V.-M., Kulmala, M., Worsnop, D. R., Wildt,
J., and Mentel, T. F.: A large source of low-volatility secondary or- ganic
aerosol, Nature, 506, 476–479, https://doi.org/10.1038/nature13032, 2014.
Guenther, A. B., Jiang, X., Heald, C. L., Sakulyanontvittaya, T., Duhl, T.,
Emmons, L. K., and Wang, X.: The Model of Emissions of Gases and Aerosols
from Nature version 2.1 (MEGAN2.1): an extended and updated framework for
modeling biogenic emissions, Geosci. Model Dev., 5, 1471–1492,
https://doi.org/10.5194/gmd-5-1471-2012, 2012.
Jimenez, J. L., Canagaratna, M. R., Donahue, N. M., Prevot, A. S. H., Zhang,
Q., Kroll, J. H., DeCarlo, P. F., Allan, J. D., Coe, H., Ng, N. L., Aiken,
A. C., Docherty, K. S., Ulbrich, I. M., Grieshop, A. P., Robinson, A. L.,
Duplissy, J., Smith, J. D., Wilson, K. R., Lanz, V. A., Hueglin, C., Sun, Y.
L., Tian, J., Laaksonen, A., Raatikainen, T., Rautiainen, J., Vaattovaara,
P., Ehn, M., Kulmala, M., Tomlinson, J. M., Collins, D. R., Cubison, M.
J., Dunlea, E. J., Huffman, J. A., Onasch, T. B., Alfarra, M. R.,
Williams, P. I., Bower, K., Kondo, Y., Schneider, J. Drewnick, F.,
Borrmann, S., Weimer, S., Demerjian, K., Salcedo, D., Cottrell, L., Griffin,
R., Takami, A., Miyoshi, T., Hatakeyama, S., Shimono, A., Sun, J. Y., Zhang,
Y. M., Dzepina, K., Kimmel, J. R., Sueper, D., Jayne, J. T., Herndon, S. C.,
Trimborn, A. M., Williams, L. R., Wood, E. C., Middlebrook, A. M., Kolb,
C. E., Baltensperger, U., and Worsnop, D. R.: Evolution of organic aerosols
in the atmosphere, Science, 326, 1525–1529,
https://doi.org/10.1126/science.1180353, 2009.
Kalberer, M., Paulsen, D., Sax, M., Steinbacher, M., Dommen, J., Prevot, A.
S. H., Fisseha, R., Weingartner, E., Frankevich, V., Zenobi, R., and
Baltensperger, U.: Identification of polymers as major components of
atmospheric organic aerosols, Science, 303, 1659–1662,
https://doi.org/10.1126/science.1092185, 2004.
Krieger, U. K., Siegrist, F., Marcolli, C., Emanuelsson, E. U., Gøbel, F. M.,
Bilde, M., Marsh, A., Reid, J. P., Huisman, A. J., Riipinen, I., Hyttinen,
N., Myllys, N., Kurtén, T., Bannan, T., Percival, C. J., and Topping, D.: A
reference data set for validating vapor pressure measurement techniques:
homologous series of polyethylene glycols, Atmos. Meas. Tech., 11, 49–63,
https://doi.org/10.5194/amt-11-49-2018, 2018.
Kurtén, T., Tiusanen, K., Roldin, P., Rissanen, M. P., Boy, M., Ehn, M.,
and Donahue, N. M. 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.
Kurtén, T., Hyttinen, N., D'Ambro, E., Thornton, J., and Prisle, N.:
Supplementary data for the manuscript “Estimating the saturation vapor pressures of isoprene
oxidation products C5H12O6 and C5H10O6 using COSMO-RS”, submitted to Atmospheric
Chemistry and Physics (Discussions) [Data set]. Zenodo, available at:
https://doi.org/10.5281/zenodo.1344890, 2018.
Liu, J., D'Ambro, E. L., Lee, B. H., Lopez-Hilfiker, F. D., Zaveri, R. A.,
Rivera-Rios, J. C., Keutsch, F. N., Iyer, S., Kurtén, T., Zhang, Z.,
Gold, A., Surratt, J. D., Shilling, J. E., and Thornton, J. A.: Efficient
Isoprene Secondary Organic Aerosol Formation from a Non-IEPOX Pathway,
Environ. Sci. Tech. Lett. 50, 9872–9880, 2016.
Lopez-Hilfiker, F. D., Mohr, C., Ehn, M., Rubach, F., Kleist, E., Wildt, J.,
Mentel, Th. F., Lutz, A., Hallquist, M., Worsnop, D., and Thornton, J. A.: A
novel method for online analysis of gas and particle composition: description
and evaluation of a Filter Inlet for Gases and AEROsols (FIGAERO), Atmos.
Meas. Tech., 7, 983–1001, https://doi.org/10.5194/amt-7-983-2014, 2014.
Nannoolal, Y., Rarey, J., and Ramjugernath, D.: Estimation of pure component
properties, Part 3, Estimation of the vapor pressure of non-electrolyte
organic compounds via group contributions and group interactions, Fluid
Phase Equilibr., 269, 117–133, 2008.
O'Meara, S., Booth, A. M., Barley, M. H., Topping, D., and McFiggans, G.: An
assessment of vapour pressure estimation methods, Phys. Chem. Chem. Phys.,
16, 19453–19469, 2014.
Pachauri, R. K. and Meyer, L. A.: Climate Change 2014: Synthesis
Report, Contribution of Working Groups I, II and III to the Fifth Assessment
Report of the Intergovernmental Panel on Climate Change, IPCC, Geneva,
Switzerland, 2014.
Pankow, J. F. and Asher, W. E.: SIMPOL.1: a simple group contribution method
for predicting vapor pressures and enthalpies of vaporization of
multifunctional organic compounds, Atmos. Chem. Phys., 8, 2773–2796,
https://doi.org/10.5194/acp-8-2773-2008, 2008.
Perdew, J. P.: Density-functional approximation for the correlation-energy
of the inhomogenous electron gas, Phys. Rev. B, 33, 8822–8824, 1986.
Pierce, J. R., Riipinen, I., Kulmala, M., Ehn, M., Petäjä, T., Junninen, H.,
Worsnop, D. R., and Donahue, N. M.: Quantification of the volatility of
secondary organic compounds in ultrafine particles during nucleation events,
Atmos. Chem. Phys., 11, 9019–9036, https://doi.org/10.5194/acp-11-9019-2011,
2011.
Puranen, J. S., Vainio, M. J., and Johnson, M. S.: Accurate
conformation-dependent molecular electrostatic potentials for
high-throughput in silico drug discovery, J. Comput. Chem., 31, 1722-1732,
https://doi.org/10.1002/jcc.21460, 2010.
TURBOMOLE V7.11: A development of University of Karlsruhe and
Forschungszentrum Karlsruhe GmbH, 1989–2007, TURBOMOLE GmbH, since 2007,
available at: http://www.turbomole.com, last access: 7 May 2018.
Vainio, M. J. and Johnson, M. S.: Generation conformer ensembles using a
multiobjective generic algorithm, J. Chem. Inf. Model., 47, 2462–2474,
https://doi.org/10.1021/ci6005646, 2007.
Valorso, R., Aumont, B., Camredon, M., Raventos-Duran, T., Mouchel-Vallon,
C., Ng, N. L., Seinfeld, J. H., Lee-Taylor, J., and Madronich, S.: Explicit
modelling of SOA formation from α-pinene photooxidation: sensitivity to
vapour pressure estimation, Atmos. Chem. Phys., 11, 6895–6910,
https://doi.org/10.5194/acp-11-6895-2011, 2011.
Wang, C., Yuan, T., Wood, S. A., Goss, K.-U., Li, J., Ying, Q., and Wania,
F.: Uncertain Henry's law constants compromise equilibrium partitioning
calculations of atmospheric oxidation products, Atmos. Chem. Phys., 17,
7529–7540, https://doi.org/10.5194/acp-17-7529-2017, 2017.
Wania, F., Lei, Y. D., Wang, C., Abbatt, J. P. D., and Goss, K.-U.: Novel
methods for predicting gas–particle partitioning during the formation of
secondary organic aerosol, Atmos. Chem. Phys., 14, 13189–13204,
https://doi.org/10.5194/acp-14-13189-2014, 2014.
Wavefunction Inc.: Spartan'14 version 1.1.9, Irvine, CA, USA, 2014.
Wennberg, P. O., Bates, K. H., Crounse, J. D., Dodson, L. G., McVay, R. C.,
Mertens, L. A., Nguyen, T. B., Praske, E., Schwantes, R. H., Smarte, M. D.,
St. Clair, J. M., Teng, A. P., Zhang, X, and Seinfeld, J. H.: Gas-Phase
Reactions of Isoprene and Its Major Oxidation Products, Chem. Rev., 118
3337-3390, https://doi.org/10.1021/acs.chemrev.7b00439, 2018.
Werner, H.-J., Knizia, G., and Manby, F. R.: Explicitly correlated coupled
cluster methods with pair-specific geminals, Mol. Phys.. 109, 407–417, 2011.
Werner, H.-J., Knowles, P. J., Knizia, G., Manby, F. R., and Schütz, M.:
Molpro: a general-purpose quantum chemistry program package, WIRES Comput.
Mol. Sci. 2, 242–253, https://doi.org/10.1002/wcms.82, 2012.
Zhang, X., Cappa, C. D., Jathar, S. H., McVay, R. C., Ensberg, J. J.,
Kleeman, M. J., and Seinfeld, J. H.: Influence of vapor wall loss in
laboratory chambers on yields of secondary organic aerosol, P. Natl.
Acad. Sci. USA, 111, 5802–5807, 2014.
Short summary
We use COSMO-RS to compute saturation vapor pressures for two products of isoprene photo-oxidation and compare the results to measurements. COSMO-RS is an attractive option for calculating properties of molecules, as it is based on quantum mechanics and requires few fitting parameters. However, we show that the default implementation of this method suffers from errors related to both conformational sampling and intramolecular hydrogen bonding. We propose solutions to these problems.
We use COSMO-RS to compute saturation vapor pressures for two products of isoprene...
Altmetrics
Final-revised paper
Preprint