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Preprints
https://doi.org/10.5194/egusphere-2024-642
https://doi.org/10.5194/egusphere-2024-642
08 Apr 2024
 | 08 Apr 2024

Cluster Dynamics-based Parameterization for Sulfuric Acid-Dimethylamine Nucleation: Comparison and Selection through Box- and Three-Dimensional- Modeling

Jiewen Shen, Bin Zhao, Shuxiao Wang, An Ning, Yuyang Li, Runlong Cai, Da Gao, Biwu Chu, Yang Gao, Manish Shrivastava, Jingkun Jiang, Xiuhui Zhang, and Hong He

Abstract. Clustering of gaseous sulfuric acid (SA) enhanced by dimethylamine (DMA) is a major mechanism for new particle formation (NPF) in polluted atmospheres. However, uncertainty remains regarding the SA-DMA nucleation parameterization that reasonably represents cluster dynamics and is applicable across various atmospheric conditions. This uncertainty hinders accurate three-dimensional (3-D) modeling of NPF and subsequent assessment of its environmental and climatic impacts. Here we extensively compare different cluster dynamics-based parameterizations for SA-DMA nucleation and identify the most reliable one through a combination of box-model simulations, 3-D modeling, and in-situ observations. Results show that the parameterization derived from Atmospheric Cluster Dynamic Code (ACDC) simulations, incorporating the latest theoretical insights (DLPNO-CCSD(T)/aug-cc-pVTZ//ωB97X-D/6-311++G(3df,3pd) level of theory) and adequate representation of cluster dynamics, exhibits dependable performance in 3-D NPF simulation for both winter and summer conditions in Beijing and shows promise for application in diverse atmospheric conditions. Another ACDC-derived parameterization, replacing the level of theory with RI-CC2/aug-cc-pV(T+d)Z//M06-2X/6–311++G(3df,3pd), also performs well in NPF modeling at relatively low temperatures around 280 K but exhibits limitations at higher temperatures due to inappropriate representation of SA-DMA cluster thermodynamics. Additionally, a previously reported parameterization incorporating simplifications is applicable for simulating NPF in polluted atmospheres but tends to overestimate particle formation rates under conditions of elevated temperature (> ~300 K) and low condensation sink (< ~3×10-3 s-1). Our findings highlight the applicability of the new ACDC-derived parameterization, which couples the latest SA-DMA nucleation theory and holistic cluster dynamics, in 3-D NPF modeling. The ACDC-derived parameterization framework provides valuable reference for developing parameterizations for other nucleation systems.

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Journal article(s) based on this preprint

18 Sep 2024
Cluster-dynamics-based parameterization for sulfuric acid–dimethylamine nucleation: comparison and selection through box and three-dimensional modeling
Jiewen Shen, Bin Zhao, Shuxiao Wang, An Ning, Yuyang Li, Runlong Cai, Da Gao, Biwu Chu, Yang Gao, Manish Shrivastava, Jingkun Jiang, Xiuhui Zhang, and Hong He
Atmos. Chem. Phys., 24, 10261–10278, https://doi.org/10.5194/acp-24-10261-2024,https://doi.org/10.5194/acp-24-10261-2024, 2024
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The requested preprint has a corresponding peer-reviewed final revised paper. You are encouraged to refer to the final revised version.

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We extensively compare various cluster-dynamics based parameterizations for sulfuric...
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