Articles | Volume 2, issue 1
https://doi.org/10.5194/ar-2-123-2024
© Author(s) 2024. 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-2-123-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
04 Jun 2024
Research article |
| 04 Jun 2024
| 04 Jun 2024
A cluster-of-functional-groups approach for studying organic enhanced atmospheric cluster formation
Astrid Nørskov Pedersen
Department of Chemistry, Aarhus University, Langelandsgade 140, 8000 Aarhus C, Denmark
Yosef Knattrup
Department of Chemistry, Aarhus University, Langelandsgade 140, 8000 Aarhus C, Denmark
Department of Chemistry, Aarhus University, Langelandsgade 140, 8000 Aarhus C, Denmark
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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.
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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.
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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
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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.
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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.
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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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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.
Aerosol formation is an important process for our global climate. While inorganic species have...
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