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Discussion papers
https://doi.org/10.5194/acp-2018-975
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2018-975
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 16 Oct 2018

Research article | 16 Oct 2018

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This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Chemistry and Physics (ACP).

Interaction between Dicarboxylic Acid and Sulfuric Acid-Base Clusters Enhances New Particle Formation

Yun Lin1, Yuemeng Ji1,2, Yixin Li1, Jeremiah Secrest1, Wen Xu3, Fei Xu4, Yuan Wang5, Taicheng An2, and Renyi Zhang1 Yun Lin et al.
  • 1Department of Atmospheric Sciences and Department of Chemistry, Texas, A&M University, College Station, TX 77843, USA
  • 2Institute of Environmental Health and Pollution Control, Guangdong University of Technology, Guangzhou 510006, China
  • 3Aerodyne Research Inc, Billerica, MA 01821, USA
  • 4School of Environmental Science and Engineering, Shandong University, Jinan 250100, China
  • 5Division of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA, 91125, USA

Abstract. Dicarboxylic acids are believed to stabilize pre-nucleation clusters and facilitate new particle formation in the atmosphere, but the detailed mechanism leading to the formation of multi-component critical nucleus involving organic acids, sulfuric acid (SA), base species, and water remains unclear. In this study, theoretical caculations are performed to elucidate the interactions between succinic acid (SUA) and clusters consisting of SA-ammonia (AM)/dimethylamine (DMA) in the presence of hydration of up to six water molecules. Formation of the hydrated SUA·SA·base clusters by adding one SUA molecule to the SA·base hydrates is energetically favorable. The addition of SUA to the SA·base hydrates either triggers proton transfer from SA to the base molecule, resulting in formation of new covalent bonds, or strengthens the pre-existing covalent bonds. The presence of SUA promotes hydration of the SA·AM and SA·AM·DMA clusters but dehydration of the SA·DMA clusters. At equilibrium, the uptake of SUA competes with the uptake of the second SA molecule to stabilize the SA·base clusters at atmospherically relevant concentrations. The clusters containing both the base and organic acid are capable of further binding with acid molecules to promote their subsequent growth. Our results indicate that the multi-component nucleation involving organic acids, sulfuric acid, and base species promotes new particle formation in the atmosphere, particularly under polluted conditions.

Yun Lin et al.
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We have investigated the molecular interactions between succinic acid and sulfuric acid·base clusters in the presence of hydration, including ammonia and dimethylamine. Our results indicate that the multi-component nucleation involving organic acids, sulfuric acid, and base species promotes new particle formation in the atmosphere, particularly under polluted conditions.
We have investigated the molecular interactions between succinic acid and sulfuric acid·base...
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