Global variability in atmospheric new particle formation mechanisms

• 成果类型: Article
• 署名作者: Zhao, Bin; Donahue, Neil M.; Zhang, Kai; Mao, Lizhuo; Shrivastava, Manish; Ma, Po-Lun; Shen, Jiewen; Wang, Shuxiao; Sun, Jian; Gordon, Hamish; Tang, Shuaiqi; Fast, Jerome; Wang, Mingyi; Gao, Yang; Yan, Chao; Singh, Balwinder; Li, Zeqi; Huang, Lyuyin; Lou, Sijia; Lin, Guangxing; Wang, Hailong; Jiang, Jingkun; Ding, Aijun; Nie, Wei; Qi, Ximeng; Chi, Xuguang; Wang, Lin
• 署名单位: Tsinghua University; United States Department of Energy (DOE); Pacific Northwest National Laboratory; Carnegie Mellon University; Carnegie Mellon University; Carnegie Mellon University; Carnegie Mellon University; National Center Atmospheric Research (NCAR) - USA; California Institute of Technology; Ocean University of China; Nanjing University; Fudan University; Xiamen University
• 刊物名称: Nature
• ISSN/ISSBN: 0028-5257
• DOI: 10.1038/s41586-024-07547-1
• 发表日期: 2024-07-04
• 页码: 98-+
• 关键词: aerosol number concentrations; volatile organic-compounds; cloud condensation nuclei; sulfuric-acid; size distributions; emissions data; gaseous methylamines; gridded emissions; upper troposphere; iodine chemistry

摘要

A key challenge in aerosol pollution studies and climate change assessment is to understand how atmospheric aerosol particles are initially formed(1,2). Although new particle formation (NPF) mechanisms have been described at specific sites(3-6), in most regions, such mechanisms remain uncertain to a large extent because of the limited ability of atmospheric models to simulate critical NPF processes(1,7). Here we synthesize molecular-level experiments to develop comprehensive representations of 11 NPF mechanisms and the complex chemical transformation of precursor gases in a fully coupled global climate model. Combined simulations and observations show that the dominant NPF mechanisms are distinct worldwide and vary with region and altitude. Previously neglected or underrepresented mechanisms involving organics, amines, iodine oxoacids and HNO3 probably dominate NPF in most regions with high concentrations of aerosols or large aerosol radiative forcing; such regions include oceanic and human-polluted continental boundary layers, as well as the upper troposphere over rainforests and Asian monsoon regions. These underrepresented mechanisms also play notable roles in other areas, such as the upper troposphere of the Pacific and Atlantic oceans. Accordingly, NPF accounts for different fractions (10-80%) of the nuclei on which cloud forms at 0.5% supersaturation over various regions in the lower troposphere. The comprehensive simulation of global NPF mechanisms can help improve estimation and source attribution of the climate effects of aerosols.