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DOI10.5194/acp-20-13109-2020
Impacts of global NOxinversions on NO2and ozone simulations
Qu Z.; Henze D.K.; Cooper O.R.; Neu J.L.
发表日期2020
ISSN16807316
起始页码13109
结束页码13130
卷号20期号:21
英文摘要Tropospheric NO2 and ozone simulations have large uncertainties, but their biases, seasonality, and trends can be improved with NO2 assimilations. We perform global top-down estimates of monthly NOx emissions using two Ozone Monitoring Instrument (OMI) NO2 retrievals (NASAv3 and DOMINOv2) from 2005 to 2016 through a hybrid 4D-Var/mass balance inversion. Discrepancy in NO2 retrieval products is a major source of uncertainties in the top-down NOx emission estimates. The different vertical sensitivities in the two NO2 retrievals affect both magnitude and seasonal variations of top-down NOx emissions. The 12-year averages of regional NOx budgets from the NASA posterior emissions are 37% to 53% smaller than the DOMINO posterior emissions. Consequently, the DOMINO posterior surface NO2 simulations greatly reduced the negative biases in China (by 15 %) and the US (by 22 %) compared to surface NO2 measurements. Posterior NOx emissions show consistent trends over China, the US, India, and Mexico constrained by the two retrievals. Emission trends are less robust over South America, Australia, western Europe, and Africa, where the two retrievals show less consistency. NO2 trends have more consistent decreases (by 26 %) with the measurements (by 32 %) in the US from 2006 to 2016 when using the NASA posterior emissions. The performance of posterior ozone simulations has spatial heterogeneities from region to region. On a global scale, ozone simulations using NASA-based emissions alleviate the double peak in the prior simulation of global ozone seasonality. The higher abundances of NO2 from the DOMINO posterior simulations increase the global background ozone concentrations and therefore reduce the negative biases more than the NASA posterior simulations using GEOS-Chem v12 at remote sites. Compared to surface ozone measurements, posterior simulations have more consistent magnitude and interannual variations than the prior estimates, but the performance from the NASA-based and DOMINO-based emissions varies across ozone metrics. The limited availability of remote-sensing data and the use of prior NOx diurnal variations hinder improvement of ozone diurnal variations from the assimilation, and therefore have mixed performance on improving different ozone metrics. Additional improvements in posterior NO2 and ozone simulations require more precise and consistent NO2 retrieval products, more accurate diurnal variations of NOx and VOC emissions, and improved simulations of ozone chemistry and depositions. © Author(s) 2020.
语种英语
scopus关键词atmospheric chemistry; atmospheric deposition; concentration (composition); diurnal variation; emission; nitrogen dioxide; ozone; seasonality; troposphere; Africa; Australia; China; India; Mexico [North America]; South America; United States; Western Europe
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/143834
作者单位Department of Mechanical Engineering, University of Colorado Boulder, Boulder, CO 80309, United States; School of Engineering and Applied Science, Harvard University, Cambridge, MA 02138, United States; Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, CO 80309, United States; NOAA Chemical Sciences Laboratory, Boulder, CO 80305, United States; Jet Propulsion Laboratory, California Institute of Technology, Pasadena, CA 91109, United States
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Qu Z.,Henze D.K.,Cooper O.R.,et al. Impacts of global NOxinversions on NO2and ozone simulations[J],2020,20(21).
APA Qu Z.,Henze D.K.,Cooper O.R.,&Neu J.L..(2020).Impacts of global NOxinversions on NO2and ozone simulations.Atmospheric Chemistry and Physics,20(21).
MLA Qu Z.,et al."Impacts of global NOxinversions on NO2and ozone simulations".Atmospheric Chemistry and Physics 20.21(2020).
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