气候变化领域集成服务门户(CCPortal): Nitrogen oxides in the free troposphere: implications for tropospheric oxidants and the interpretation of satellite NO2 measurements

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DOI	10.5194/acp-23-1227-2023
	Nitrogen oxides in the free troposphere: implications for tropospheric oxidants and the interpretation of satellite NO2 measurements
	Shah, Viral; Jacob, Daniel J.; Dang, Ruijun; Lamsal, Lok N.; Strode, Sarah A.; Steenrod, Stephen D.; Boersma, K. Folkert; Eastham, Sebastian D.; Fritz, Thibaud M.; Thompson, Chelsea; Peischl, Jeff; Bourgeois, Ilann; Pollack, Ilana B.; Nault, Benjamin A.; Cohen, Ronald C.; Campuzano-Jost, Pedro; Jimenez, Jose L.; Andersen, Simone T.; Carpenter, Lucy J.; Sherwen, Tomas; Evans, Mat J.
发表日期	2023
ISSN	1680-7316
EISSN	1680-7324
起始页码	1227
结束页码	1257
卷号	23 期号:2 页码:31
英文摘要	Satellite-based retrievals of tropospheric NO(2)columns are widely used to infer NOx (equivalent to NO + NO2) emissions. These retrievals rely on model information for the vertical distribution of NO2. The free tropospheric background above 2 km is particularly important because the sensitivity of the retrievals increases with altitude. Free tropospheric NOx also has a strong effect on tropospheric OH and ozone concentrations. Here we use observations from three aircraft campaigns (SEAC(4)RS, DC3, and ATom) and four atmospheric chemistry models (GEOS-Chem, GMI, TM5, and CAMS) to evaluate the model capabilities for simulating NOx in the free troposphere and attribute it to sources. NO2 measurements during the Studies of Emissions and Atmospheric Composition, Clouds, and Climate Coupling by Regional Surveys (SEAC4RS) and Deep Convective Clouds and Chemistry (DC3) campaigns over the southeastern U.S. in summer show increasing concentrations in the upper troposphere above 10 km, which are not replicated by the GEOS-Chem, although the model is consistent with the NO measurements. Using concurrent NO, NO2, and ozone observations from a DC3 flight in a thunderstorm outflow, we show that the NO2 measurements in the upper troposphere are biased high, plausibly due to interference from thermally labile NO(2)reservoirs such as peroxynitric acid (HNO4) and methyl peroxy nitrate (MPN). We find that NO2 concentrations calculated from the NO measurements and NO-NO2 photochemical steady state (PSS) are more reliable to evaluate the vertical profiles of NO2 in models. GEOS-Chem reproduces the shape of the PSS-inferred NO2 profiles throughout the troposphere for SEAC(4)RS and DC3 but overestimates NO2 concentrations by about a factor of 2. The model underestimates MPN and alkyl nitrate concentrations, suggesting missing organic NOx chemistry. On the other hand, the standard GEOS-Chem model underestimates NO observations from the Atmospheric Tomography Mission (ATom) campaigns over the Pacific and Atlantic oceans, indicating a missing NOx source over the oceans. We find that we can account for this missing source by including in the model the photolysis of particulate nitrate on sea salt aerosols at rates inferred from laboratory studies and field observations of nitrous acid (HONO) over the Atlantic. The median PSS-inferred tropospheric NO2 column density for the ATom campaign is 1.7 +/- 0.44 x 10(14) molec. cm(-2), and the NO2 column density simulated by the four models is in the range of 1.4-2.4 x 10(14) molec. cm(-2), implying that the uncertainty from using modeled NO2 tropospheric columns over clean areas in the retrievals for stratosphere-troposphere separation is about 1 x 10(14 )molec. cm(-2). We find from GEOS-Chem that lightning is the main primary NOx source in the free troposphere over the tropics and southern midlatitudes, but aircraft emissions dominate at northern midlatitudes in winter and in summer over the oceans. Particulate nitrate photolysis increases ozone concentrations by up to 5 ppbv (parts per billion by volume) in the free troposphere in the northern extratropics in the model, which would largely correct the low model bias relative to ozonesonde observations. Global tropospheric OH concentrations increase by 19 %. The contribution of the free tropospheric background to the tropospheric NO2 columns observed by satellites over the contiguous U.S. increases from 25 +/- 11 % in winter to 65 +/- 9 % in summer, according to the GEOS-Chem vertical profiles. This needs to be accounted for when deriving NOx emissions from satellite NO2 column measurements.
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:000921909300001
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/273248
作者单位	Harvard University; Harvard University; National Aeronautics & Space Administration (NASA); University System of Maryland; University of Maryland Baltimore County; Morgan State University; Royal Netherlands Meteorological Institute; Wageningen University & Research; Massachusetts Institute of Technology (MIT); Massachusetts Institute of Technology (MIT); University of Colorado System; University of Colorado Boulder; Colorado State University; Aerodyne Research; University of California System; University of California Berkeley; University of California System; University of California Berkeley; University of Colorado System; University of Colorado Boulder; University of Colorado System; University of Colorado Boulder; University of York - UK; UK Research & Innovation (UKRI); Natural Environment Research Council (NERC); NERC National Centre for Atmospheric Science; University of York - UK; National Aeronautics & Space Administration (NASA); NASA Goddard Space Flight Center; Science Systems and Applications...
推荐引用方式 GB/T 7714	Shah, Viral,Jacob, Daniel J.,Dang, Ruijun,et al. Nitrogen oxides in the free troposphere: implications for tropospheric oxidants and the interpretation of satellite NO2 measurements[J],2023,23(2):31.
APA	Shah, Viral.,Jacob, Daniel J..,Dang, Ruijun.,Lamsal, Lok N..,Strode, Sarah A..,...&Evans, Mat J..(2023).Nitrogen oxides in the free troposphere: implications for tropospheric oxidants and the interpretation of satellite NO2 measurements.ATMOSPHERIC CHEMISTRY AND PHYSICS,23(2),31.
MLA	Shah, Viral,et al."Nitrogen oxides in the free troposphere: implications for tropospheric oxidants and the interpretation of satellite NO2 measurements".ATMOSPHERIC CHEMISTRY AND PHYSICS 23.2(2023):31.