气候变化领域集成服务门户(CCPortal): Unraveling the diurnal atmospheric ammonia budget of a prototypical convective boundary layer

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DOI	10.1016/j.atmosenv.2020.118153
	Unraveling the diurnal atmospheric ammonia budget of a prototypical convective boundary layer
	Schulte R.B.; van Zanten M.C.; Rutledge-Jonker S.; Swart D.P.J.; Wichink Kruit R.J.; Krol M.C.; van Pul W.A.J.; Vilà-Guerau de Arellano J.
发表日期	2021
ISSN	1352-2310
卷号	249
英文摘要	We investigate diurnal variability of the atmospheric ammonia (NH3) budget over unfertilized grassland by combining observations with a conceptual atmospheric boundary layer model. Our combined approach of diurnal observations and modeling enables us to identify the contribution of the four governing processes to the NH3 diurnal cycle: surface-atmosphere exchange, entrainment, advection and chemical gas-aerosol transformations. The observations contain new NH3 flux and molar fraction measurements obtained using the Differential Optical Absorption Spectroscopy (DOAS) remote sensing technique, eliminating problems related to inlet tubing. Using strict filter criteria, 22 days with clear-sky summer conditions are selected. From this selection, we analyze a single representative day characterized by prototypical convective boundary layer conditions, using the boundary layer model constrained by meteorological observations. We design two numerical experiments to study the NH3 diurnal variability and the individual contributions of the processes governing the ammonia budget. These experiments only differ in their representation of the NH3 surface exchange. First, a fitted function through the observed NH3 flux is prescribed to the model. In the second numerical experiment, the surface flux is solved following the DEPosition of Acidifying Compounds (DEPAC) parameterization. With a prescribed surface flux, the modeled NH3 molar fraction closely fits the observations. Two regimes are identified in the NH3 diurnal cycle: the morning, where boundary layer dynamics dominate the budget through entrainment, and the afternoon, where multiple processes are of importance. A similarly close fit to the observed molar fraction is achieved in the second experiment, but we identify a mismatch between the observed and parameterized NH3 surface flux. As a result, the model requires an unrealistic budget representation to achieve this close fit, e.g. high free tropospheric NH3. Our findings on the NH3 budget, based on integrating modeling and observations, paves the way for future research on the NH3 surface-atmosphere exchange at the subdaily scales. © 2021 The Authors
关键词	Ammonia Budget Convective boundary layer Diurnal variability Modeling. measurements
语种	英语
scopus关键词	Absorption spectroscopy; Atmospheric boundary layer; Atmospheric chemistry; Boundary layer flow; Budget control; Light absorption; Remote sensing; Surface measurement; Acidifying compounds; Boundary layer dynamics; Boundary layer models; Convective boundary layers; Differential optical absorption spectroscopy; Meteorological observation; Numerical experiments; Remote sensing techniques; Ammonia; ammonia; nitrogen; ammonia; boundary layer; convective boundary layer; filter; numerical model; parameterization; remote sensing; absorption spectroscopy; advection; aerosol; air temperature; Article; atmosphere; boundary layer; budget; circadian rhythm; concentration (parameter); controlled study; gas; grassland; growing season; meteorological phenomena; optics; priority journal; prototypical convective boundary layer; remote sensing; soil temperature; species composition; summer; surface property; troposphere; turbulent flow; water vapor; wind speed
来源期刊	ATMOSPHERIC ENVIRONMENT
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/248546
作者单位	Wageningen University & Research, P.O. Box 47, AA Wageningen, 6700, Netherlands; National Institute for Public Health and the Environment (RIVM), Antonie van Leeuwenhoeklaan 9, MA Bilthoven, 3721, Netherlands
推荐引用方式 GB/T 7714	Schulte R.B.,van Zanten M.C.,Rutledge-Jonker S.,et al. Unraveling the diurnal atmospheric ammonia budget of a prototypical convective boundary layer[J],2021,249.
APA	Schulte R.B..,van Zanten M.C..,Rutledge-Jonker S..,Swart D.P.J..,Wichink Kruit R.J..,...&Vilà-Guerau de Arellano J..(2021).Unraveling the diurnal atmospheric ammonia budget of a prototypical convective boundary layer.ATMOSPHERIC ENVIRONMENT,249.
MLA	Schulte R.B.,et al."Unraveling the diurnal atmospheric ammonia budget of a prototypical convective boundary layer".ATMOSPHERIC ENVIRONMENT 249(2021).