气候变化领域集成服务门户(CCPortal): Effects of Ozone Isotopologue Formation on the Clumped-Isotope Composition of Atmospheric O2

CCPortal

DOI	10.1029/2021JD034770
	Effects of Ozone Isotopologue Formation on the Clumped-Isotope Composition of Atmospheric O2
	Yeung L.Y.; Murray L.T.; Banerjee A.; Tie X.; Yan Y.; Atlas E.L.; Schauffler S.M.; Boering K.A.
发表日期	2021
ISSN	2169-897X
卷号	126 期号:14
英文摘要	Tropospheric 18O18O is an emerging proxy for past tropospheric ozone and free-tropospheric temperatures. The basis of these applications is the idea that isotope-exchange reactions in the atmosphere drive 18O18O abundances toward isotopic equilibrium. However, previous work used an offline box-model framework to explain the 18O18O budget, approximating the interplay of atmospheric chemistry and transport. This approach, while convenient, has poorly characterized uncertainties. To investigate these uncertainties, and to broaden the applicability of the 18O18O proxy, we developed a scheme to simulate atmospheric 18O18O abundances (quantified as ∆36 values) online within the GEOS-Chem chemical transport model. These results are compared to both new and previously published atmospheric observations from the surface to 33 km. Simulations using a simplified O2 isotopic equilibration scheme within GEOS-Chem show quantitative agreement with measurements only in the middle stratosphere; modeled ∆36 values are too high elsewhere. Investigations using a comprehensive model of the O-O2-O3 isotopic photochemical system and proof-of-principle experiments suggest that the simple equilibration scheme omits an important pressure dependence to ∆36 values: the anomalously efficient titration of 18O18O to form ozone. Incorporating these effects into the online ∆36 calculation scheme in GEOS-Chem yields quantitative agreement for all available observations. While this previously unidentified bias affects the atmospheric budget of 18O18O in O2, the modeled change in the mean tropospheric ∆36 value since 1850 CE is only slightly altered; it is still quantitatively consistent with the ice-core ∆36 record, implying that the tropospheric ozone burden increased less than 40% over the twentieth century. © 2021. American Geophysical Union. All Rights Reserved.
英文关键词	clumped isotopes; GEOS-Chem; oxygen; ozone; preindustrial; stratosphere-troposphere exchange
来源期刊	Journal of Geophysical Research: Atmospheres
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/237164
作者单位	Department of Earth, Environmental and Planetary Sciences, Rice University, Houston, TX, United States; Department of Earth and Environmental Sciences, University of Rochester, Rochester, NY, United States; Division of Marine and Atmospheric Chemistry, University of Miami, Miami, FL, United States; National Center for Atmospheric Research, Boulder, CO, United States; Departments of Chemistry and Earth and Planetary Science, University of California, Berkeley, CA, United States
推荐引用方式 GB/T 7714	Yeung L.Y.,Murray L.T.,Banerjee A.,et al. Effects of Ozone Isotopologue Formation on the Clumped-Isotope Composition of Atmospheric O2[J],2021,126(14).
APA	Yeung L.Y..,Murray L.T..,Banerjee A..,Tie X..,Yan Y..,...&Boering K.A..(2021).Effects of Ozone Isotopologue Formation on the Clumped-Isotope Composition of Atmospheric O2.Journal of Geophysical Research: Atmospheres,126(14).
MLA	Yeung L.Y.,et al."Effects of Ozone Isotopologue Formation on the Clumped-Isotope Composition of Atmospheric O2".Journal of Geophysical Research: Atmospheres 126.14(2021).