31 Jan 2023
 | 31 Jan 2023
Status: this preprint is currently under review for the journal ACP.

A parameterization of sulfuric acid-dimethylamine nucleation and its application in three-dimensional modeling

Yuyang Li, Jiewen Shen, Bin Zhao, Runlong Cai, Shuxiao Wang, Yang Gao, Manish Shrivastava, Da Gao, Jun Zheng, Markku Kulmala, and Jingkun Jiang

Abstract. Sulfuric acid (SA) is a governing gaseous precursor for atmospheric new particle formation (NPF) in diverse environments, which is a major source of global ultrafine particles. In polluted urban atmosphere with high condensation sink (CS), the formation of stable SA-amine clusters, such as SA-DMA clusters, usually initializes intense NPF events. Coagulation scavenging and cluster evaporation are dominant sink processes of SA-amine clusters in urban atmosphere, yet they are not quantitatively included in the present parameterizations of SA-amine nucleation. We herein report a parameterization of SA-DMA nucleation based on cluster dynamic simulations and quantum chemistry calculations, with certain simplifications to largely reduce the computational costs. Compared with previous SA-DMA nucleation parameterizations, this new parameterization would be able to reproduce the dependences of particle formation rates on temperature and CS. We then incorporated it in a three-dimensional chemical transport model to simulate the evolution of particle number size distributions. Simulation results show good consistency with the observations in the occurrence of NPF events and particle number size distributions in wintertime Beijing, showing a significant improvement compared to that using parameterization without coagulation scavenging. Quantitative analysis shows that SA-DMA nucleation contributes majorly to nucleation rates and aerosol population during the 3-D simulations in Beijing (> 99 % and > 60 %, respectively). These results broaden the understanding of NPF in urban atmospheres and stress the necessity of including the effects of coagulation scavenging and cluster stability in simulating SA-DMA nucleation in three-dimensional simulations. This would improve the performance in particle source apportionment and quantification of aerosol effects on air quality, human health, and climate.

Yuyang Li et al.

Status: open (until 28 Mar 2023)

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  • RC1: 'Comment on acp-2023-15', Anonymous Referee #1, 19 Feb 2023 reply

Yuyang Li et al.


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Short summary
We set up a new parameterization for 1.4 nm particle formation rates from sulfuric acid (SA)-dimethylamine (DMA) nucleation, fully including the effects of coagulation scavenging and cluster stability. Incorporating the new parameterization into a 3-D chemical transport models, we achieved better consistencies between simulation results and observation data. This new parameterization provides new insights into atmospheric nucleation simulations and its effects on atmospheric pollution or health.