气候变化领域集成服务门户(CCPortal): Diurnal evolution of total column and surface atmospheric ammonia in the megacity of Paris, France, during an intense springtime pollution episode

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DOI	10.5194/acp-21-12091-2021
	Diurnal evolution of total column and surface atmospheric ammonia in the megacity of Paris, France, during an intense springtime pollution episode
	Kutzner R.D.; Cuesta J.; Chelin P.; Petit J.-E.; Ray M.; Landsheere X.; Tournadre B.; Dupont J.-C.; Rosso A.; Hase F.; Orphal J.; Beekmann M.
发表日期	2021
ISSN	1680-7316
起始页码	12091
结束页码	12111
卷号	21 期号:15
英文摘要	Ammonia (NH3) is a key precursor for the formation of atmospheric secondary inorganic particles, such as ammonium nitrate and sulfate. Although the chemical processes associated with the gas-to-particle conversion are well known, atmospheric concentrations of gaseous ammonia are still scarcely characterized. However, this information is critical, especially for processes concerning the equilibrium between ammonia and ammonium nitrate, due to the semivolatile character of the latter. This study presents an analysis of the diurnal cycle of atmospheric ammonia during a pollution event over the Paris megacity region in spring 2012 (5gd in late March 2012). Our objective is to analyze the link between the diurnal evolution of surface NH3 concentrations and its integrated column abundance, meteorological variables and relevant chemical species involved in gas-particle partitioning. For this, we implement an original approach based on the combined use of surface and total column ammonia measurements. These last ones are derived from ground-based remote sensing measurements performed by the Observations of the Atmosphere by Solar Infrared Spectroscopy (OASIS) Fourier transform infrared observatory at an urban site over the southeastern suburbs of the Paris megacity. This analysis considers the following meteorological variables and processes relevant to the ammonia pollution event: temperature, relative humidity, wind speed and direction, and the atmospheric boundary layer height (as indicator of vertical dilution during its diurnal development). Moreover, we study the partitioning between ammonia and ammonium particles from concomitant measurements of total particulate matter (PM) and ammonium (NH4+) concentrations at the surface. We identify the origin of the pollution event as local emissions at the beginning of the analyzed period and advection of pollution from Benelux and western Germany by the end. Our results show a clearly different diurnal behavior of atmospheric ammonia concentrations at the surface and those vertically integrated over the total atmospheric column. Surface concentrations remain relatively stable during the day, while total column abundances show a minimum value in the morning and rise steadily to reach a relative maximum in the late afternoon during each day of the spring pollution event. These differences are mainly explained by vertical mixing within the boundary layer, provided that this last one is considered well mixed and therefore homogeneous in ammonia concentrations. This is suggested by ground-based measurements of vertical profiles of aerosol backscatter, used as tracer of the vertical distribution of pollutants in the atmospheric boundary layer. Indeed, the afternoon enhancement of ammonia clearly seen by OASIS for the whole atmospheric column is barely depicted by surface concentrations, as the surface concentrations are strongly affected by vertical dilution within the rising boundary layer. Moreover, the concomitant occurrence of a decrease in ammonium particle concentrations and an increase in gaseous ammonia abundance suggests the volatilization of particles for forming ammonia. Furthermore, surface observations may also suggest nighttime formation of ammonium particles from gas-to-particle conversion, for relative humidity levels higher than the deliquescence point of ammonium nitrate. © 2021 The Author(s)..
语种	英语
scopus关键词	ammonia; atmospheric pollution; boundary layer; concentration (composition); diurnal variation; megacity; spring (season); France; Ile de France; Paris; Ville de Paris; Indicator indicator
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/246659
作者单位	Laboratoire Interuniversitaire des Systèmes Atmosphériques (LISA), Umr Cnrs 7583, Université Paris-Est Créteil, Université de Paris, Institut Pierre-Simon Laplace (IPSL), Créteil, France; Laboratoire des Sciences du Climat et de l'Environnement, Umr 8212, CEA/Orme des Merisiers, Gif-sur-Yvette, 91191, France; Ineris, Parc Technologique Alata, Verneuil-en-Halatte, 60750, France; Institut Pierre-Simon Laplace, École Polytechnique Uvsq, Université Paris-Saclay, Palaiseau, 91128, France; Airparif Agence de Surveillance de la Qualité de l'Air, Paris, France; Institut für Meteorologie und Klimaforschung (IMK), Karlsruher Institut für Technologie (KIT), Karlsruhe, Germany; Centre Observation, Impacts, Energy - Mines ParisTech, Sophia Antipolis Cedex, France
推荐引用方式 GB/T 7714	Kutzner R.D.,Cuesta J.,Chelin P.,et al. Diurnal evolution of total column and surface atmospheric ammonia in the megacity of Paris, France, during an intense springtime pollution episode[J],2021,21(15).
APA	Kutzner R.D..,Cuesta J..,Chelin P..,Petit J.-E..,Ray M..,...&Beekmann M..(2021).Diurnal evolution of total column and surface atmospheric ammonia in the megacity of Paris, France, during an intense springtime pollution episode.ATMOSPHERIC CHEMISTRY AND PHYSICS,21(15).
MLA	Kutzner R.D.,et al."Diurnal evolution of total column and surface atmospheric ammonia in the megacity of Paris, France, during an intense springtime pollution episode".ATMOSPHERIC CHEMISTRY AND PHYSICS 21.15(2021).