Contribution of Methanesulfonic Acid to the Formation of Molecular Clusters in the Marine Atmosphere

Freja Rydahl Rasmussen, Jakub Kubecka, Jonas Elm*

*Corresponding author af dette arbejde

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Abstract

Because of the lack of long-term measurements, new particle formation (NPF) in the marine atmosphere remains puzzling. Using quantum chemical methods, this study elucidates the cluster formation and further growth of sulfuric acid-methanesulfonic acid-dimethylamine (SA-MSA-DMA) clusters, relevant to NPF in the marine atmosphere. The cluster structures and thermochemical parameters of (SA) n(MSA) m(DMA) l(n + m ≤ 4 and l ≤ 4) systems are calculated using density functional theory at the ωB97X-D/6-31++G(d,p) level of theory, and the single-point energies are calculated using high-level DLPNO-CCSD(T 0)/aug-cc-pVTZ calculations. The calculated thermochemistry is used as input to the Atmospheric Cluster Dynamics Code (ACDC) to gain insight into the cluster dynamics. At ambient conditions (298.15 K, 1 atm), we find that the distribution of outgrowing clusters primarily consists of SA and DMA, with a minor contribution from the mixed SA-MSA-DMA clusters. At lower temperature (278.15 K, 1 atm) the distribution broadens, and clusters containing one or more MSA molecules emerge. These findings show that in the cold marine atmosphere MSA likely participates in atmospheric NPF.

OriginalsprogEngelsk
TidsskriftThe Journal of Physical Chemistry A
Vol/bind126
Nummer40
Sider (fra-til)7127–7136
Antal sider10
ISSN1089-5639
DOI
StatusUdgivet - okt. 2022

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