Experiment-theory hybrid method for studying the formation mechanism of atmospheric new particle formation
文献类型：期刊论文
| 作者 | Liu, Yi-Rong2 ; Jiang, Shuai2; Huang, Teng1; Zhang, Fan2
|
| 刊名 | PHYSICAL CHEMISTRY CHEMICAL PHYSICS
 |
| 出版日期 | 2022-11-23 |
| 卷号 | 24 |
| ISSN号 | 1463-9076 |
| DOI | 10.1039/d2cp03551k |
| 通讯作者 | Liu, Yi-Rong(yrliu@ustc.edu.cn) |
| 英文摘要 | Atmospheric aerosols have a significant influence on climate change through their effect on the cloud lifetime and the radiative balance of the Earth's atmosphere. Despite its importance, the mechanism of aerosol nucleation is still poorly understood. Based on the low-energy structure of cluster molecules, quantum chemical (QC) computations can help us to directly calculate the formation mechanism of atmospheric clusters and formation rates at the molecular level. However, deciphering the formation mechanism of pre-nucleated clusters, especially those close to the critical size (similar to 1.7 nm), remains extremely challenging because many millions of configuration spaces might need to be explored to find the low-energy structure. We present a new idea that establishes a comprehensive experimental and computational hybrid calculation protocol to integrate experimental data, isomer distributions, hydrogen bond interactions, and interaction sites for exploring the configuration spaces and clarifying the nucleation mechanism of acid-base clusters, whose maximum size can exceed 1.7 nm. This protocol can effectively and accurately explore the configuration space of complex large nucleation clusters on the potential energy surface (PES). The consistency of the cluster concentration and the formation rate between the experiment and the in situ measurement is much better than that of the previous studies and proves its accuracy. In addition, we found that malic acid (MA) can enhance sulfuric acid-dimethylamine (SA-DMA)-based particle formation rates in the atmospheric boundary layer, for example, in Shanghai and Beijing in the summer, with an enhancement of up to 700- and 135-fold, respectively. The enhancement in atmospheric particle formation by MA is critical for new particle formation in the boundary layer with relatively low SA and DMA concentrations and at high temperature. This model greatly improves our understanding of the complex aerosol nucleation mechanism of large-scale multicomponent cluster molecules. |
| WOS关键词 | SULFURIC-ACID ; AEROSOL FORMATION ; NUCLEATION ; AMINES ; DIMETHYLAMINE ; DYNAMICS ; GROWTH ; MODEL ; WATER |
| 资助项目 | National Natural Science Foundation of China ; [41775112] ; [41877305] |
| WOS研究方向 | Chemistry ; Physics |
| 语种 | 英语 |
| WOS记录号 | WOS:000883662600001 |
| 出版者 | ROYAL SOC CHEMISTRY |
| 资助机构 | National Natural Science Foundation of China |
| 源URL | [http://ir.hfcas.ac.cn:8080/handle/334002/130118]  |
| 专题 | 中国科学院合肥物质科学研究院 |
| 通讯作者 | Liu, Yi-Rong |
| 作者单位 | 1.Chinese Acad Sci, Anhui Inst Opt & Fine Mech, Lab Atmospher Physico Chem, Hefei 230031, Anhui, Peoples R China 2.Univ Sci & Technol China, Sch Informat Sci & Technol, Hefei 230026, Anhui, Peoples R China |
| 推荐引用方式 GB/T 7714 | Liu, Yi-Rong,Jiang, Shuai,Huang, Teng,et al. Experiment-theory hybrid method for studying the formation mechanism of atmospheric new particle formation[J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS,2022,24. |
| APA | Liu, Yi-Rong,Jiang, Shuai,Huang, Teng,&Zhang, Fan.(2022).Experiment-theory hybrid method for studying the formation mechanism of atmospheric new particle formation.PHYSICAL CHEMISTRY CHEMICAL PHYSICS,24. |
| MLA | Liu, Yi-Rong,et al."Experiment-theory hybrid method for studying the formation mechanism of atmospheric new particle formation".PHYSICAL CHEMISTRY CHEMICAL PHYSICS 24(2022). |
入库方式： OAI收割
来源：合肥物质科学研究院
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