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DOI10.5194/acp-21-13729-2021
Heterogeneity and chemical reactivity of the remote troposphere defined by aircraft measurements
Guo H.; Flynn C.M.; Prather M.J.; Strode S.A.; Steenrod S.D.; Emmons L.; Lacey F.; Lamarque J.-F.; Fiore A.M.; Correa G.; Murray L.T.; Wolfe G.M.; St. Clair J.M.; Kim M.; Crounse J.; Diskin G.; Digangi J.; Daube B.C.; Commane R.; Mckain K.; Peischl J.; Ryerson T.B.; Thompson C.; Hanisco T.F.; Blake D.; Blake N.J.; Apel E.C.; Hornbrook R.S.; Elkins J.W.; Hintsa E.J.; Moore F.L.; Wofsy S.
发表日期2021
ISSN1680-7316
起始页码13729
结束页码13746
卷号21期号:18
英文摘要The NASA Atmospheric Tomography (ATom) mission built a photochemical climatology of air parcels based on in situ measurements with the NASA DC-8 aircraft along objectively planned profiling transects through the middle of the Pacific and Atlantic oceans. In this paper we present and analyze a data set of 10s (2km) merged and gap-filled observations of the key reactive species driving the chemical budgets of O3 and CH4 (O3, CH4, CO, H2O, HCHO, H2O2, CH3OOH, C2H6, higher alkanes, alkenes, aromatics, NOx, HNO3, HNO4, peroxyacetyl nitrate, other organic nitrates), consisting of 146494 distinct air parcels from ATom deployments 1 through 4. Six models calculated the O3 and CH4 photochemical tendencies from this modeling data stream for ATom 1. We find that 80%-90% of the total reactivity lies in the top 50% of the parcels and 25%-35% in the top 10%, supporting previous model-only studies that tropospheric chemistry is driven by a fraction of all the air. In other words, accurate simulation of the least reactive 50% of the troposphere is unimportant for global budgets. Surprisingly, the probability densities of species and reactivities averaged on a model scale (100km) differ only slightly from the 2km ATom data, indicating that much of the heterogeneity in tropospheric chemistry can be captured with current global chemistry models. Comparing the ATom reactivities over the tropical oceans with climatological statistics from six global chemistry models, we find excellent agreement with the loss of O3 and CH4 but sharp disagreement with production of O3. The models sharply underestimate O3 production below 4km in both Pacific and Atlantic basins, and this can be traced to lower NOx levels than observed. Attaching photochemical reactivities to measurements of chemical species allows for a richer, yet more constrained-to-what-matters, set of metrics for model evaluation. © 2021 Hao Guo et al.
语种英语
scopus关键词airborne survey; atmospheric chemistry; data set; heterogeneity; methane; ozone; troposphere
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/246578
作者单位Department of Earth System Science, University of California, Irvine, CA 92697, United States; Department of Meteorology, Stockholm University, Stockholm, 10691, Sweden; Atmospheric Chemistry and Dynamics Laboratory, NASA Goddard Space Flight Center, Greenbelt, MD 20771, United States; Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder, CO 80301, United States; Department of Mechanical Engineering, University of Colorado, Boulder, CO 80309, United States; Department of Earth and Environmental Sciences, Lamont-Doherty Earth Observatory, Columbia University, Palisades, NY 10964, United States; Department of Earth and Environmental Sciences, University of Rochester, Rochester, NY 14611, United States; Joint Center for Earth Systems Technology, University of Maryland, Baltimore County, Baltimore, MD 21228, United States; Department of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA 91125, United States; Atmo...
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Guo H.,Flynn C.M.,Prather M.J.,et al. Heterogeneity and chemical reactivity of the remote troposphere defined by aircraft measurements[J],2021,21(18).
APA Guo H..,Flynn C.M..,Prather M.J..,Strode S.A..,Steenrod S.D..,...&Wofsy S..(2021).Heterogeneity and chemical reactivity of the remote troposphere defined by aircraft measurements.ATMOSPHERIC CHEMISTRY AND PHYSICS,21(18).
MLA Guo H.,et al."Heterogeneity and chemical reactivity of the remote troposphere defined by aircraft measurements".ATMOSPHERIC CHEMISTRY AND PHYSICS 21.18(2021).
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