The role of hydration in atmospheric salt particle formation

Myllys, Nanna

doi:10.1039/d3cp00049d

Cited by 4 publications

(2 citation statements)

References 64 publications

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“…Highly oxygenated molecules (HOMs) are also important for NPF, but to date, there is little information about the exact structure of relevant HOMs . Finally, water should also be taken into account to accurately model different relative humidity conditions. − …”

Section: Resultsmentioning

confidence: 99%

Nitric Acid and Organic Acids Suppress the Role of Methanesulfonic Acid in Atmospheric New Particle Formation

Knattrup,

Kubečka,

Elm

2023

J. Phys. Chem. A

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Multicomponent atmospheric molecular clusters, typically comprising a combination of acids and bases, play a pivotal role in our climate system and contribute to the perplexing uncertainties embedded in modern climate models. Our understanding of cluster formation is limited by the lack of studies on complex mixed-acid–mixed-base systems. Here, we investigate multicomponent clusters consisting of mixtures of several acid and base molecules: sulfuric acid (SA), methanesulfonic acid (MSA), nitric acid (NA), formic acid (FA), along with methylamine (MA), dimethylamine (DMA), and trimethylamine (TMA). We calculated the binding free energies of a comprehensive set of 252 mixed-acid–mixed-base clusters at the DLPNO–CCSD(T0)/aug-cc-pVTZ//ωB97X-D/6-31++G(d,p) level of theory. Combined with the existing datasets, we simulated the new particle formation (NPF) rates using the Atmospheric Cluster Dynamics Code (ACDC). We find that the presence of NA and FA had a substantial impact, increasing the NPF rate by 60% at realistic conditions. Intriguingly, we find that NA and FA suppress the role of MSA in NPF. These findings suggest that even high concentration of MSA has a limited impact on NPF in polluted regions with high FA and NA. We outline a method for generating a lookup table that could potentially be used in climate models that sufficiently incorporates all the required chemistry. By unraveling the molecular mechanisms of mixed-acid–mixed-base clusters, we get one step closer to comprehending their implications for our global climate system.

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Section: Resultsmentioning

confidence: 99%

Nitric Acid and Organic Acids Suppress the Role of Methanesulfonic Acid in Atmospheric New Particle Formation

Knattrup,

Kubečka,

Elm

2023

J. Phys. Chem. A

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“…8–14 Thus, an incredible amount of experimental and computational effort has been devoted to understanding which species are involved, and how they combine together, to form secondary aerosols. 6,8–85 It is common in the field to work under the assumption that acids and bases grow into an ensemble that contains an equal number of both types of molecules. 8–14 Yet, the tremendous number of potential compounds that can form prenucleation clusters is vast, and there is no experimental technique that can identify all of the different molecules in prenucleation complexes or small aerosols in the sub-nanometer (nm) to nm size range.…”

Section: Introductionmentioning

confidence: 99%

The driving effects of common atmospheric molecules for formation of clusters: the case of sulfuric acid, nitric acid, hydrochloric acid, ammonia, and dimethylamine

Longsworth,

Bready,

Joines

et al. 2023

Environ. Sci.: Atmos.

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Quantum chemical modeling of atmospheric molecular clusters involving inorganic acids and methanesulfonic acid

Engsvang,

Wu,

Knattrup

et al. 2023

Chemical Physics Reviews

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Atmospheric molecular cluster formation is the first stage toward aerosol particle formation. Despite intensive progress in recent years, the relative role of different vapors and the mechanisms for forming clusters is still not well-understood. Quantum chemical (QC) methods can give insight into the cluster formation mechanisms and thereby yield information about the potentially relevant compounds. Here, we summarize the QC literature on clustering involving species such as sulfuric acid, methanesulfonic acid, and nitric acid. The importance of iodine species such as iodous acid (HIO2) and iodic acid (HIO3) in atmospheric cluster formation is an emerging topic, and we critically review the recent literature and give our view on how to progress in the future. We outline how machine learning (ML) methods can be used to enhance cluster configurational sampling, leading to a massive increase in the cluster compositions that can be modeled. In the future, ML-boosted cluster formation could allow us to comprehensively understand complex cluster formation with multiple pathways, leading us one step closer to implementing accurate cluster formation mechanisms in atmospheric models.

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The role of hydration in atmospheric salt particle formation

Abstract: New-particle formation from condensable acid and base molecules is a ubiquitous phenomenon in the atmosphere. The role of water in the salt particle formation is not fully understood as it...

Cited by 4 publications

References 64 publications

Nitric Acid and Organic Acids Suppress the Role of Methanesulfonic Acid in Atmospheric New Particle Formation

Nitric Acid and Organic Acids Suppress the Role of Methanesulfonic Acid in Atmospheric New Particle Formation

The driving effects of common atmospheric molecules for formation of clusters: the case of sulfuric acid, nitric acid, hydrochloric acid, ammonia, and dimethylamine

Quantum chemical modeling of atmospheric molecular clusters involving inorganic acids and methanesulfonic acid

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