气候变化领域集成服务门户(CCPortal): Fundamental oxidation processes in the remote marine atmosphere investigated using the NO-NO2-O-3 photostationary state

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DOI	10.5194/acp-22-15747-2022
	Fundamental oxidation processes in the remote marine atmosphere investigated using the NO-NO2-O-3 photostationary state
	Andersen, Simone T.; Nelson, Beth S.; Read, Katie A.; Punjabi, Shalini; Neves, Luis; Rowlinson, Matthew J.; Hopkins, James; Sherwen, Tomas; Whalley, Lisa K.; Lee, James D.; Carpenter, Lucy J.
发表日期	2022
ISSN	1680-7316
EISSN	1680-7324
起始页码	15747
结束页码	15765
卷号	22 期号:24 页码:19
英文摘要	The photostationary state (PSS) equilibrium between NO and NO2 is reached within minutes in the atmosphere and can be described by the PSS parameter, phi. Deviations from expected values of phi have previously been used to infer missing oxidants in diverse locations, from highly polluted regions to the extremely clean conditions observed in the remote marine boundary layer (MBL), and have been interpreted as missing understanding of fundamental photochemistry. Here, contrary to these previous observations, we observe good agreement between PSS-derived NO2 ([NO2](PSS) (ext.)), calculated from measured NO, O-3, and jNO(2) and photochemical box model predictions of peroxy radicals (RO2 and HO2), and observed NO2 ([NO2](Obs.)) in extremely clean air containing low levels of CO (< 90 ppbV) and VOCs (volatile organic compounds). However, in clean air containing small amounts of aged pollution (CO > 100 ppbV), we observed higher levels of NO2 than inferred from the PSS, with [NO2](Obs.) / [NO2](PSS ext.) of 1.12-1.68 (25th-75th percentile), implying underestimation of RO2 radicals by 18.5-104 pptV. Potential NO2 measurement artefacts have to be carefully considered when comparing PSS-derived NO2 to observed NO2, but we show that the NO2 artefact required to explain the deviation would have to be similar to 4 times greater than the maximum calculated from known interferences. If the additional RO2 radicals inferred from the PSS convert NO to NO2 with a reaction rate equivalent to that of methyl peroxy radicals (CH3O2), then the calculated net ozone production rate (NOPR, ppbV h(-1)) including these additional oxidants is similar to the average change in O-3 observed, within estimated uncertainties, once halogen oxide chemistry is accounted for. This implies that such additional peroxy radicals cannot be excluded as a missing oxidant in clean marine air containing aged pollution and that modelled RO2 concentrations are significantly underestimated under these conditions.
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:000899238100001
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/273911
作者单位	University of York - UK; University of York - UK; University of Leeds
推荐引用方式 GB/T 7714	Andersen, Simone T.,Nelson, Beth S.,Read, Katie A.,et al. Fundamental oxidation processes in the remote marine atmosphere investigated using the NO-NO2-O-3 photostationary state[J],2022,22(24):19.
APA	Andersen, Simone T..,Nelson, Beth S..,Read, Katie A..,Punjabi, Shalini.,Neves, Luis.,...&Carpenter, Lucy J..(2022).Fundamental oxidation processes in the remote marine atmosphere investigated using the NO-NO2-O-3 photostationary state.ATMOSPHERIC CHEMISTRY AND PHYSICS,22(24),19.
MLA	Andersen, Simone T.,et al."Fundamental oxidation processes in the remote marine atmosphere investigated using the NO-NO2-O-3 photostationary state".ATMOSPHERIC CHEMISTRY AND PHYSICS 22.24(2022):19.