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DOI	10.5194/acp-22-8579-2022
	Influence of emission size distribution and nucleation on number concentrations over Greater Paris
	Sartelet, Karine; Kim, Youngseob; Couvidat, Florian; Merkel, Maik; Petaja, Tuukka; Sciare, Jean; Wiedensohler, Alfred
发表日期	2022
ISSN	1680-7316
EISSN	1680-7324
起始页码	8579
结束页码	8596
卷号	22 期号:13 页码:18
英文摘要	With the growing evidence that high particle number concentrations may impact health, modelling their emissions and understanding formation processes is necessary, especially in cities where many people are exposed. As emission inventories of particle numbers and size distribution over cities are usually not available, a methodology is defined to estimate them from PM2.5 emissions and ratios of PM1 / PM2.5 and PM0.1 / PM2.5 by activity sector. In this methodology, a fitting parameter alpha(em) is used to redistribute the number concentrations in the lowest emission diameter range. This parameter is chosen by comparing measured and simulated number concentrations during non-nucleation days. The emission size distribution is then finely discretised by conserving both mass and number in each of the size ranges where emissions are specified. The methodology is applied over Greater Paris during the MEGAPOLI campaign (July 2009). Three-dimensional simulations are performed using the chemistry transport model Polair3D/Polyphemus coupled to the aerosol module SSH-aerosol to represent the evolution of particles by condensation, evaporation, coagulation, and nucleation, with a sectional approach for the size distribution. The model is first compared to measurements during non-nucleation days, and the influence over the month of July 2009 of three different nucleation parameterisations is assessed, i.e. binary (sulfuric acid, water), ternary (sulfuric acid, ammonia, water), and heteromolecular (extremely low-volatility organic compounds (ELVOCs) from monoterpenes and sulfuric acid). The modelled number concentrations compare very well to measurements, with an average normalised mean error of 42 % for the daily number concentrations of particles larger than 10 nm and 37 % for the number concentrations of particles larger than 100 nm. The influence of the binary nucleation is low, and the ternary nucleation scheme leads to better simulated number concentrations (in terms of bias and error) at only one site out of three, but it systematically reduces the model to measurement correlation, suggesting that ternary nucleation may not be the dominant process in new particle formation. However, the relative bias and error, as well as the correlation at suburban sites, are systematically improved using the heteromolecular nucleation scheme involving sulfuric acid and ELVOCs from monoterpenes. This suggests that heteromolecular nucleation may be important in cities, especially at suburban sites in summer, and that a better characterisation of the emissions of ELVOC precursors from traffic is needed.
学科领域	Environmental Sciences; Meteorology & Atmospheric Sciences
语种	英语
WOS研究方向	Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences
WOS记录号	WOS:000820740300001
来源期刊	ATMOSPHERIC CHEMISTRY AND PHYSICS
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/273885
作者单位	Ecole des Ponts ParisTech; Electricite de France (EDF); Leibniz Institut fur Tropospharenforschung (TROPOS); University of Helsinki; UDICE-French Research Universities; Universite Paris Saclay; CEA; Centre National de la Recherche Scientifique (CNRS)
推荐引用方式 GB/T 7714	Sartelet, Karine,Kim, Youngseob,Couvidat, Florian,et al. Influence of emission size distribution and nucleation on number concentrations over Greater Paris[J],2022,22(13):18.
APA	Sartelet, Karine.,Kim, Youngseob.,Couvidat, Florian.,Merkel, Maik.,Petaja, Tuukka.,...&Wiedensohler, Alfred.(2022).Influence of emission size distribution and nucleation on number concentrations over Greater Paris.ATMOSPHERIC CHEMISTRY AND PHYSICS,22(13),18.
MLA	Sartelet, Karine,et al."Influence of emission size distribution and nucleation on number concentrations over Greater Paris".ATMOSPHERIC CHEMISTRY AND PHYSICS 22.13(2022):18.