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DOI	10.1073/pnas.2006716117
	High concentration of ultrafine particles in the Amazon free troposphere produced by organic new particle formation
	Zhao B.; Shrivastava M.; Donahue N.M.; Gordon H.; Schervish M.; Shilling J.E.; Zaveri R.A.; Wang J.; Andreae M.O.; Zhao C.; Gaudet B.; Liu Y.; Fan J.; Fast J.D.
发表日期	2020
ISSN	0027-8424
起始页码	25344
结束页码	25351
卷号	117 期号:41
英文摘要	The large concentrations of ultrafine particles consistently observed at high altitudes over the tropics represent one of the world's largest aerosol reservoirs, which may be providing a globally important source of cloud condensation nuclei. However, the sources and chemical processes contributing to the formation of these particles remain unclear. Here we investigate new particle formation (NPF) mechanisms in the Amazon free troposphere by integrating insights from laboratory measurements, chemical transport modeling, and field measurements. To account for organic NPF, we develop a comprehensive model representation of the temperature-dependent formation chemistry and thermodynamics of extremely low volatility organic compounds as well as their roles in NPF processes. We find that pure-organic NPF driven by natural biogenic emissions dominates in the uppermost troposphere above 13 km and accounts for 65 to 83% of the column total NPF rate under relatively pristine conditions, while ternary NPF involving organics and sulfuric acid dominates between 8 and 13 km. The large organic NPF rates at high altitudes mainly result from decreased volatility of organics and increased NPF efficiency at low temperatures, somewhat counterbalanced by a reduced chemical formation rate of extremely low volatility organic compounds. These findings imply a key role of naturally occurring organic NPF in high-altitude preindustrial environments and will help better quantify anthropogenic aerosol forcing from preindustrial times to the present day. © 2020 National Academy of Sciences. All rights reserved.
英文关键词	Aerosol; Amazon; Extremely low volatility organic compounds; New particle formation; Troposphere
语种	英语
scopus关键词	sulfuric acid; Article; autooxidation; bioaccumulation; concentration (parameter); controlled study; dimerization; new particle formation; priority journal; quantum chemistry; room temperature; secondary organic aerosol; simulation; thermodynamics; troposphere; ultrafine particulate matter
来源期刊	Proceedings of the National Academy of Sciences of the United States of America
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/160769
作者单位	Zhao, B., Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland, WA 99352, United States; Shrivastava, M., Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland, WA 99352, United States; Donahue, N.M., Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA 15213, United States, Department of Chemistry, Carnegie Mellon University, Pittsburgh, PA 15213, United States, Department of Engineering and Public Policy, Carnegie Mellon University, Pittsburgh, PA 15213, United States, Department of Chemical Engineering, Carnegie Mellon University, Pittsburgh, PA 15213, United States; Gordon, H., Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA 15213, United States, School of Earth and Environment, University of Leeds, Leeds, LS2 9JT, United Kingdom; Schervish, M., Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA 15213, United ...
推荐引用方式 GB/T 7714	Zhao B.,Shrivastava M.,Donahue N.M.,et al. High concentration of ultrafine particles in the Amazon free troposphere produced by organic new particle formation[J],2020,117(41).
APA	Zhao B..,Shrivastava M..,Donahue N.M..,Gordon H..,Schervish M..,...&Fast J.D..(2020).High concentration of ultrafine particles in the Amazon free troposphere produced by organic new particle formation.Proceedings of the National Academy of Sciences of the United States of America,117(41).
MLA	Zhao B.,et al."High concentration of ultrafine particles in the Amazon free troposphere produced by organic new particle formation".Proceedings of the National Academy of Sciences of the United States of America 117.41(2020).