气候变化领域集成服务门户(CCPortal): Characterization of organic aerosol across the global remote troposphere: A comparison of ATom measurements and global chemistry models

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DOI	10.5194/acp-20-4607-2020
	Characterization of organic aerosol across the global remote troposphere: A comparison of ATom measurements and global chemistry models
	Hodzic A.; Campuzano-Jost P.; Bian H.; Chin M.; Colarco P.R.; Day D.A.; Froyd K.D.; Heinold B.; Jo D.S.; Katich J.M.; Kodros J.K.; Nault B.A.; Pierce J.R.; Ray E.; Schacht J.; Schill G.P.; Schroder J.C.; Schwarz J.P.; Sueper D.T.; Tegen I.; Tilmes S.; Tsigaridis K.; Yu P.; Jimenez J.L.
发表日期	2020
ISSN	1680-7316
起始页码	4607
结束页码	4635
卷号	20 期号:8
英文摘要	The spatial distribution and properties of submicron organic aerosol (OA) are among the key sources of uncertainty in our understanding of aerosol effects on climate. Uncertainties are particularly large over remote regions of the free troposphere and Southern Ocean, where very few data have been available and where OA predictions from AeroCom Phase II global models span 2 to 3 orders of magnitude, greatly exceeding the model spread over source regions. The (nearly) pole-to-pole vertical distribution of nonrefractory aerosols was measured with an aerosol mass spectrometer onboard the NASA DC-8 aircraft as part of the Atmospheric Tomography (ATom) mission during the Northern Hemisphere summer (August 2016) and winter (February 2017). This study presents the first extensive characterization of OA mass concentrations and their level of oxidation in the remote atmosphere. OA and sulfate are the major contributors by mass to submicron aerosols in the remote troposphere, together with sea salt in the marine boundary layer. Sulfate was dominant in the lower stratosphere. OA concentrations have a strong seasonal and zonal variability, with the highest levels measured in the lower troposphere in the summer and over the regions influenced by biomass burning from Africa (up to 10 μgsm-3). Lower concentrations (~ 0:1 0.3 μgsm-3) are observed in the northern middle and high latitudes and very low concentrations (< 0:1 μgsm-3) in the southern middle and high latitudes. The ATom dataset is used to evaluate predictions of eight current global chemistry models that implement a variety of commonly used representations of OA sources and chemistry, as well as of the AeroCom-II ensemble. The current model ensemble captures the average vertical and spatial distribution of measured OA concentrations, and the spread of the individual models remains within a factor of 5. These results are significantly improved over the AeroCom-II model ensemble, which shows large overestimations over these regions. However, some of the improved agreement with observations occurs for the wrong reasons, as models have the tendency to greatly overestimate the primary OA fraction and underestimate the sec-ondary fraction. Measured OA in the remote free troposphere is highly oxygenated, with organic aerosol to organic carbon (OA= OC) ratios of ~ 2.2 2.8, and is 30 % 60% more oxygenated than in current models, which can lead to significant errors in OA concentrations. The model measurement comparisons presented here support the concept of a more dynamic OA system as proposed by Hodzic et al. (2016), with enhanced removal of primary OA and a stronger production of secondary OA in global models needed to provide better agreement with observations. © 2020 IEEE Computer Society. All rights reserved.
语种	英语
scopus关键词	aerosol composition; aerosol formation; mass spectrometry; Northern Hemisphere; numerical model; spatial distribution; troposphere; uncertainty analysis
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/141396
作者单位	National Center for Atmospheric Research, Boulder, CO, United States; Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado, Boulder, CO, United States; Department of Chemistry, University of Colorado, Boulder, CO, United States; NASA Goddard Space Flight Center, Greenbelt, MD, United States; NOAA Earth System Research Laboratory (ESRL), Chemical Sciences Division, Boulder, CO, United States; Department of Atmospheric Science, Colorado State University, Fort Collins, CO, United States; Leibniz Institute for Tropospheric Research, Leipzig, Germany; Center for Climate Systems Research, Columbia University, New York, NY, United States; NASA Goddard Institute for Space Studies, New York, NY, United States; Institute for Environmental and Climate Research, Jinan University, Guangzhou, Guangdong, China
推荐引用方式 GB/T 7714	Hodzic A.,Campuzano-Jost P.,Bian H.,et al. Characterization of organic aerosol across the global remote troposphere: A comparison of ATom measurements and global chemistry models[J],2020,20(8).
APA	Hodzic A..,Campuzano-Jost P..,Bian H..,Chin M..,Colarco P.R..,...&Jimenez J.L..(2020).Characterization of organic aerosol across the global remote troposphere: A comparison of ATom measurements and global chemistry models.Atmospheric Chemistry and Physics,20(8).
MLA	Hodzic A.,et al."Characterization of organic aerosol across the global remote troposphere: A comparison of ATom measurements and global chemistry models".Atmospheric Chemistry and Physics 20.8(2020).