Articles | Volume 22, issue 17
https://doi.org/10.5194/acp-22-11543-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-22-11543-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
07 Sep 2022
Research article |
| 07 Sep 2022
| 07 Sep 2022
Atmospheric oxidation mechanism and kinetics of indole initiated by ●OH and ●Cl: a computational study
Jingwen Xue
Key Laboratory of Industrial Ecology and Environmental Engineering
(Ministry of Education), School of Environmental Science and Technology,
Dalian University of Technology, Dalian 116024, China
Fangfang Ma
CORRESPONDING AUTHOR
Key Laboratory of Industrial Ecology and Environmental Engineering
(Ministry of Education), School of Environmental Science and Technology,
Dalian University of Technology, Dalian 116024, China
Jonas Elm
Department of Chemistry and iClimate, Aarhus University,
Langelandsgade 140, 8000 Aarhus C, Denmark
Jingwen Chen
Key Laboratory of Industrial Ecology and Environmental Engineering
(Ministry of Education), School of Environmental Science and Technology,
Dalian University of Technology, Dalian 116024, China
Hong-Bin Xie
CORRESPONDING AUTHOR
Key Laboratory of Industrial Ecology and Environmental Engineering
(Ministry of Education), School of Environmental Science and Technology,
Dalian University of Technology, Dalian 116024, China
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Astrid Nørskov Pedersen, Yosef Knattrup, and Jonas Elm
Aerosol Research Discuss., https://doi.org/10.5194/ar-2026-10, https://doi.org/10.5194/ar-2026-10, 2026
Preprint under review for AR
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We investigated the new particle formation (NPF) potential of three atmospherically relevant oxygenated organic molecules (OOMs) using high-level computational methods. Cluster thermodynamics and formation rates were evaluated for systems containing sulfuric acid and various nitrogen bases. All three OOMs enhanced cluster formation, with dimethylamine-containing clusters showing the greatest effect. PDPE formed the most stable clusters, due to its molecular flexibility.
Qian Xu, Fangfang Ma, Chang Liu, Qiaojing Zhao, Jingwen Chen, and Hong-Bin Xie
Atmos. Chem. Phys., 26, 3211–3222, https://doi.org/10.5194/acp-26-3211-2026, https://doi.org/10.5194/acp-26-3211-2026, 2026
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·Cl-initiated oxidation of imines was investigated to clarify their atmospheric fate and reaction mechanisms. This study revealed that NH-containing imines mainly yield N-centered radicals, which react with NO to form nitrosamines or with O2 to form cyanide compounds, with pathways strongly dependent on molecular structure of N-centered radicals. This results highlight the role of imines in nitrosamine formation and advance Cl/ONCs chemistry.
Ivo Neefjes, Jakub Kubečka, and Jonas Elm
EGUsphere, https://doi.org/10.5194/egusphere-2026-696, https://doi.org/10.5194/egusphere-2026-696, 2026
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Atmospheric particles impact climate and health. Most particles form through gas molecules colliding and sticking together. We use molecular dynamics accelerated by machine learning to study this process. We found that standard machine learning models often fail to capture the long-range forces driving collisions, and models with explicit long-range corrections are needed. This work provides a blueprint for accurate simulations of particle formation.
Ivo Neefjes, Yosef Knattrup, Haide Wu, Georg Baadsgaard Trolle, Jonas Elm, and Jakub Kubečka
Aerosol Research, 4, 1–22, https://doi.org/10.5194/ar-4-1-2026, https://doi.org/10.5194/ar-4-1-2026, 2026
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We investigated how water vapor affects the earliest steps of atmospheric aerosol formation, a key process influencing clouds and climate. By benchmarking quantum-chemical methods, we identified reliable approaches for modeling hydrated molecular clusters of common atmospheric acids and bases. We show that humidity moderately stabilizes certain clusters but only modestly alters particle formation rates. These findings sharpen our understanding of clusters and their role in aerosol formation.
Qiaojing Zhao, Fangfang Ma, Hui Zhao, Qian Xu, Rujing Yin, Hong-Bin Xie, Xin Wang, and Jingwen Chen
Atmos. Chem. Phys., 25, 12615–12628, https://doi.org/10.5194/acp-25-12615-2025, https://doi.org/10.5194/acp-25-12615-2025, 2025
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The scarcity of kinetic data for key aerosol aqueous-phase reactions contributes to large uncertainties in atmospheric models. We establish a computational strategy to rapidly predict acid-catalyzed hydrolysis kinetics of organic hydroperoxides, an aerosol constituent with high abundance. The kinetic parameters can be integrated into atmospheric models to improve simulations of the global hydrogen peroxide budget and secondary organic aerosol production.
Tenglong Shi, Jiayao Wang, Daizhou Zhang, Jiecan Cui, Zihang Wang, Yue Zhou, Wei Pu, Yang Bai, Zhigang Han, Meng Liu, Yanbiao Liu, Hongbin Xie, Minghui Yang, Ying Li, Meng Gao, and Xin Wang
The Cryosphere, 19, 2821–2835, https://doi.org/10.5194/tc-19-2821-2025, https://doi.org/10.5194/tc-19-2821-2025, 2025
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This study examines the properties of dust in snow in Changchun, China, using advanced technology to analyze its size, shape, and light absorption. We found that dust composition affects how much heat is absorbed by snow, with certain minerals, such as hematite, making snowmelt faster. Our research highlights the importance of creating clear standards for classifying dust, which could improve climate models and field observations. This work helps better understand dust's role in climate change.
Yosef Knattrup, Ivo Neefjes, Jakub Kubečka, and Jonas Elm
Aerosol Research, 3, 237–251, https://doi.org/10.5194/ar-3-237-2025, https://doi.org/10.5194/ar-3-237-2025, 2025
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Aerosols, a large uncertainty in climate modeling, can be formed when gas vapors and particles begin sticking together. Traditionally, these particles are assumed to behave like hard spheres that only stick together upon head-on collisions. In reality, particles can attract each other over distances, leading to more frequent sticking events. We found that traditional models significantly undercount these events, with real sticking rates being up to 2.4 times higher.
Yosef Knattrup and Jonas Elm
Aerosol Research, 3, 125–137, https://doi.org/10.5194/ar-3-125-2025, https://doi.org/10.5194/ar-3-125-2025, 2025
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Using quantum chemical methods, we studied the uptake of first-generation oxidation products onto freshly nucleated particles (FNPs). We find that pinic acid can condense on these small FNPs at realistic atmospheric conditions, thereby contributing to early particle growth. The mechanism involves two pinic acid molecules interacting with each other, showing that direct organic–organic interactions during co-condensation onto the particle contribute to the growth.
Galib Hasan, Haide Wu, Yosef Knattrup, and Jonas Elm
Aerosol Research, 3, 101–111, https://doi.org/10.5194/ar-3-101-2025, https://doi.org/10.5194/ar-3-101-2025, 2025
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Aerosol formation is an important process for our global climate. However, there are high uncertainties associated with the formation of new aerosol particles. We present quantum chemical calculations of large atmospheric molecular clusters composed of sulfuric acid (SA), ammonia (AM), and dimethylamine (DMA). We find that mixed SA–AM–DMA systems cluster more efficiently for freshly nucleated particles compared to pure SA–AM and SA–DMA systems.
Haide Wu, Yosef Knattrup, Andreas Buchgraitz Jensen, and Jonas Elm
Aerosol Research, 2, 303–314, https://doi.org/10.5194/ar-2-303-2024, https://doi.org/10.5194/ar-2-303-2024, 2024
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The exact point at which a given assembly of molecules represents an atmospheric molecular cluster or a particle remains ambiguous. Using quantum chemical methods, here we explore a cluster-to-particle transition point. Based on our results, we deduce a property-based criterion for defining freshly nucleated particles (FNPs) that act as a boundary between discrete cluster configurations and bulk particles.
Astrid Nørskov Pedersen, Yosef Knattrup, and Jonas Elm
Aerosol Research, 2, 123–134, https://doi.org/10.5194/ar-2-123-2024, https://doi.org/10.5194/ar-2-123-2024, 2024
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Aerosol formation is an important process for our global climate. While inorganic species have been shown to be important for aerosol formation, there remains a large gap in our knowledge about the exact involvement of organics. We present a new quantum chemical procedure for screening relevant organics that for the first time allows us to obtain direct molecular-level insight into the organics involved in aerosol formation.
Zhiqiang Zhang, Ying Li, Haiyan Ran, Junling An, Yu Qu, Wei Zhou, Weiqi Xu, Weiwei Hu, Hongbin Xie, Zifa Wang, Yele Sun, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 4809–4826, https://doi.org/10.5194/acp-24-4809-2024, https://doi.org/10.5194/acp-24-4809-2024, 2024
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Secondary organic aerosols (SOAs) can exist in liquid, semi-solid, or amorphous solid states, which are rarely accounted for in current chemical transport models. We predict the phase state of SOA particles over China and find that in northwestern China SOA particles are mostly highly viscous or glassy solid. Our results indicate that the particle phase state should be considered in SOA formation in chemical transport models for more accurate prediction of SOA mass concentrations.
Jonas Elm, Aladár Czitrovszky, Andreas Held, Annele Virtanen, Astrid Kiendler-Scharr, Benjamin J. Murray, Daniel McCluskey, Daniele Contini, David Broday, Eirini Goudeli, Hilkka Timonen, Joan Rosell-Llompart, Jose L. Castillo, Evangelia Diapouli, Mar Viana, Maria E. Messing, Markku Kulmala, Naděžda Zíková, and Sebastian H. Schmitt
Aerosol Research, 1, 13–16, https://doi.org/10.5194/ar-1-13-2023, https://doi.org/10.5194/ar-1-13-2023, 2023
Bernadette Rosati, Sini Isokääntä, Sigurd Christiansen, Mads Mørk Jensen, Shamjad P. Moosakutty, Robin Wollesen de Jonge, Andreas Massling, Marianne Glasius, Jonas Elm, Annele Virtanen, and Merete Bilde
Atmos. Chem. Phys., 22, 13449–13466, https://doi.org/10.5194/acp-22-13449-2022, https://doi.org/10.5194/acp-22-13449-2022, 2022
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Sulfate aerosols have a strong influence on climate. Due to the reduction in sulfur-based fossil fuels, natural sulfur emissions play an increasingly important role. Studies investigating the climate relevance of natural sulfur aerosols are scarce. We study the water uptake of such particles in the laboratory, demonstrating a high potential to take up water and form cloud droplets. During atmospheric transit, chemical processing affects the particles’ composition and thus their water uptake.
Rongjie Zhang, Jiewen Shen, Hong-Bin Xie, Jingwen Chen, and Jonas Elm
Atmos. Chem. Phys., 22, 2639–2650, https://doi.org/10.5194/acp-22-2639-2022, https://doi.org/10.5194/acp-22-2639-2022, 2022
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Formic acid is screened out as the species that can effectively catalyze the new particle formation (NPF) of the methanesulfonic acid (MSA)–methylamine system, indicating organic acids might be required to facilitate MSA-driven NPF in the atmosphere. The results are significant to comprehensively understand the MSA-driven NPF and expand current knowledge of the contribution of OAs to NPF.
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
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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.
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Short summary
·OH/·Cl initiated indole reactions mainly form organonitrates, alkoxy radicals and hydroperoxide products, showing a varying mechanism from previously reported amines reactions. This study reveals carcinogenic nitrosamines cannot be formed in indole oxidation reactions despite radicals formed from -NH- H abstraction. The results are important to understand the atmospheric impact of indole oxidation and extend current understanding on the atmospheric chemistry of organic nitrogen compounds.
·OH/·Cl initiated indole reactions mainly form organonitrates, alkoxy radicals and...
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