Articles | Volume 3, issue 1
https://doi.org/10.5194/ar-3-125-2025
© Author(s) 2025. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/ar-3-125-2025
© Author(s) 2025. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
28 Feb 2025
Research article |
| 28 Feb 2025
| 28 Feb 2025
Uptake of organic vapours and nitric acid on atmospheric freshly nucleated particles
Yosef Knattrup
Department of Chemistry, Aarhus University, Langelandsgade 140, 8000 Aarhus C, Denmark
Department of Chemistry, Aarhus University, Langelandsgade 140, 8000 Aarhus C, Denmark
Related authors
Yosef Knattrup, Ivo Neefjes, Jakub Kubecka, and Jonas Elm
Aerosol Research Discuss., https://doi.org/10.5194/ar-2025-9, https://doi.org/10.5194/ar-2025-9, 2025
Preprint under review for AR
Short summary
Short summary
Aerosols, a large uncertainty in climate modeling, can be formed when gas vapors and particles begin sticking together. Traditionally, these particles are assumed to behave like hard spheres that only stick together upon head on collisions. In reality, particles can attract each other over distances, leading to more frequent sticking events. We found that traditional models significantly undercount these events, with real sticking rates being up to 2.4 times higher.
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
Short summary
Short summary
Aerosol formation is an important process for our global climate. While inorganic species have been shown to be important for aerosol formation, there remains a large gap in our knowledge about the exact involvement of organics. We present a new quantum chemical procedure for screening relevant organics that for the first time allows us to obtain direct molecular-level insight into the organics involved in aerosol formation.
Yosef Knattrup, Ivo Neefjes, Jakub Kubecka, and Jonas Elm
Aerosol Research Discuss., https://doi.org/10.5194/ar-2025-9, https://doi.org/10.5194/ar-2025-9, 2025
Preprint under review for AR
Short summary
Short summary
Aerosols, a large uncertainty in climate modeling, can be formed when gas vapors and particles begin sticking together. Traditionally, these particles are assumed to behave like hard spheres that only stick together upon head on collisions. In reality, particles can attract each other over distances, leading to more frequent sticking events. We found that traditional models significantly undercount these events, with real sticking rates being up to 2.4 times higher.
Galib Hasan, Haide Wu, Yosef Knattrup, and Jonas Elm
Aerosol Research, 3, 101–111, https://doi.org/10.5194/ar-3-101-2025, https://doi.org/10.5194/ar-3-101-2025, 2025
Short summary
Short summary
Aerosol formation is an important process for our global climate. However, there are high uncertainties associated with the formation of new aerosol particles. We present quantum chemical calculations of large atmospheric molecular clusters composed of sulfuric acid (SA), ammonia (AM), and dimethylamine (DMA). We find that mixed SA–AM–DMA systems cluster more efficiently for freshly nucleated particles compared to pure SA–AM and SA–DMA systems.
Haide Wu, Yosef Knattrup, Andreas Buchgraitz Jensen, and Jonas Elm
Aerosol Research, 2, 303–314, https://doi.org/10.5194/ar-2-303-2024, https://doi.org/10.5194/ar-2-303-2024, 2024
Short summary
Short summary
The exact point at which a given assembly of molecules represents an atmospheric molecular cluster or a particle remains ambiguous. Using quantum chemical methods, here we explore a cluster-to-particle transition point. Based on our results, we deduce a property-based criterion for defining freshly nucleated particles (FNPs) that act as a boundary between discrete cluster configurations and bulk particles.
Astrid Nørskov Pedersen, Yosef Knattrup, and Jonas Elm
Aerosol Research, 2, 123–134, https://doi.org/10.5194/ar-2-123-2024, https://doi.org/10.5194/ar-2-123-2024, 2024
Short summary
Short summary
Aerosol formation is an important process for our global climate. While inorganic species have been shown to be important for aerosol formation, there remains a large gap in our knowledge about the exact involvement of organics. We present a new quantum chemical procedure for screening relevant organics that for the first time allows us to obtain direct molecular-level insight into the organics involved in aerosol formation.
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.
Jingwen Xue, Fangfang Ma, Jonas Elm, Jingwen Chen, and Hong-Bin Xie
Atmos. Chem. Phys., 22, 11543–11555, https://doi.org/10.5194/acp-22-11543-2022, https://doi.org/10.5194/acp-22-11543-2022, 2022
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·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.
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.
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
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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.
Kasper Kristensen, Louise N. Jensen, Lauriane L. J. Quéléver, Sigurd Christiansen, Bernadette Rosati, Jonas Elm, Ricky Teiwes, Henrik B. Pedersen, Marianne Glasius, Mikael Ehn, and Merete Bilde
Atmos. Chem. Phys., 20, 12549–12567, https://doi.org/10.5194/acp-20-12549-2020, https://doi.org/10.5194/acp-20-12549-2020, 2020
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Atmospheric particles are important in relation to human health and the global climate. As the global temperature changes, so may the atmospheric chemistry controlling the formation of particles from reactions of naturally emitted volatile organic compounds (VOCs). In the current work, we show how temperatures influence the formation and chemical composition of atmospheric particles from α-pinene: a biogenic VOC largely emitted in high-latitude environments such as the boreal forests.
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
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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.
Related subject area
Fundamental Aerosol Research (FAR)
The impact of unimolecular reactions on acyl peroxy radical initiated isoprene oxidation
Base synergy in freshly nucleated particles
Particle deliquescence in a turbulent humidity field
Cluster-to-particle transition in atmospheric nanoclusters
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A cluster-of-functional-groups approach for studying organic enhanced atmospheric cluster formation
Photocatalytic chloride-to-chlorine conversion by ionic iron in aqueous aerosols: a combined experimental, quantum chemical, and chemical equilibrium model study
Ida Karppinen, Dominika Pasik, Emelda Ahongshangbam, and Nanna Myllys
Aerosol Research, 3, 175–183, https://doi.org/10.5194/ar-3-175-2025, https://doi.org/10.5194/ar-3-175-2025, 2025
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Acyl peroxy radicals can act as atmospheric oxidants of unsaturated hydrocarbons if their 1) unimolecular reactions are slow and 2) bimolecular accretion reactions are fast. Using theoretical tools, we show which acyl peroxy radicals should be considered oxidants in the atmosphere.
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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.
Dennis Niedermeier, Rasmus Hoffmann, Silvio Schmalfuss, Wiebke Frey, Fabian Senf, Olaf Hellmuth, Mira Pöhlker, and Frank Stratmann
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Revised manuscript accepted for AR
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This study examines the deliquescence behavior of NaCl particles in a turbulent humidity field using the wind tunnel LACIS-T. The results show turbulent relative humidity (RH) fluctuations affect the number of deliquesced particles, depending on mean RH, strength of humidity fluctuations, and particle residence time. It turns out that, in addition to the mean RH, it is essential to consider humidity fluctuations and particle history when determining the phase state of the deliquescent particles.
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.
Anindya Ganguly, Khaled Mosharraf Mukut, Somesh Roy, Georgios Kelesidis, and Eirini Goudeli
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Revised manuscript accepted for AR
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The study explores the formation of small soot clusters by precursor molecules at high temperature. Higher temperature speeds up the decomposition of gas molecules, accelerating the formation of cyclic structures decorated by aliphatic chains. This research offers new insights into the early steps of soot formation, which could help develop more informed kinetic models for pyrolysis and combustion processes.
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We analyze the mechanism whereby sunlight and iron catalyze the production of chlorine from chloride in sea spray aerosol. This process occurs naturally over the North Atlantic and is the single most important source of chlorine. We investigate the mechanism using quantum chemistry, laboratory experiments, and aqueous chemistry modelling. The process will change depending on competing ions, light distribution, acidity, and chloride concentration.
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Short summary
Using quantum chemical methods, we studied the uptake of first-generation oxidation products onto freshly nucleated particles (FNPs). We find that pinic acid can condense on these small FNPs at realistic atmospheric conditions, thereby contributing to early particle growth. The mechanism involves two pinic acid molecules interacting with each other, showing that direct organic–organic interactions during co-condensation onto the particle contribute to the growth.
Using quantum chemical methods, we studied the uptake of first-generation oxidation products...
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