气候变化领域集成服务门户(CCPortal): Inverse modelling of carbonyl sulfide: Implementation, evaluation and implications for the global budget

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DOI	10.5194/acp-21-3507-2021
	Inverse modelling of carbonyl sulfide: Implementation, evaluation and implications for the global budget
	Ma J.; Kooijmans L.M.J.; Cho A.; Montzka S.A.; Glatthor N.; Worden J.R.; Kuai L.; Atlas E.L.; Krol M.C.
发表日期	2021
ISSN	1680-7316
起始页码	3507
结束页码	3529
卷号	21 期号:5
英文摘要	Carbonyl sulfide (COS) has the potential to be used as a climate diagnostic due to its close coupling to the biospheric uptake of CO2 and its role in the formation of stratospheric aerosol. The current understanding of the COS budget, however, lacks COS sources, which have previously been allocated to the tropical ocean. This paper presents a first attempt at global inverse modelling of COS within the 4-dimensional variational data-assimilation system of the TM5 chemistry transport model (TM5-4DVAR) and a comparison of the results with various COS observations. We focus on the global COS budget, including COS production from its precursors carbon disulfide (CS2) and dimethyl sulfide (DMS). To this end, we implemented COS uptake by soil and vegetation from an updated biosphere model (Simple Biosphere Model-SiB4). In the calculation of these fluxes, a fixed atmospheric mole fraction of 500 pmol mol-1 was assumed. We also used new inventories for anthropogenic and biomass burning emissions. The model framework is capable of closing the COS budget by optimizing for missing emissions using NOAA observations in the period 2000-2012. The addition of 432 Gg a-1 (as S equivalents) of COS is required to obtain a good fit with NOAA observations. This missing source shows few year-to-year variations but considerable seasonal variations. We found that the missing sources are likely located in the tropical regions, and an overestimated biospheric sink in the tropics cannot be ruled out due to missing observations in the tropical continental boundary layer. Moreover, high latitudes in the Northern Hemisphere require extra COS uptake or reduced emissions. HIPPO (HIAPER Pole-to-Pole Observations) aircraft observations, NOAA airborne profiles from an ongoing monitoring programme and several satellite data sources are used to evaluate the optimized model results. This evaluation indicates that COS mole fractions in the free troposphere remain underestimated after optimization. Assimilation of HIPPO observations slightly improves this model bias, which implies that additional observations are urgently required to constrain sources and sinks of COS. We finally find that the biosphere flux dependency on the surface COS mole fraction (which was not accounted for in this study) may substantially lower the fluxes of the SiB4 biosphere model over strong-uptake regions. Using COS mole fractions from our inversion, the prior biosphere flux reduces from 1053 to 851 Gg a-1, which is closer to 738 Gg a-1 as was found by Berry et al. (2013). In planned further studies we will implement this biosphere dependency and additionally assimilate satellite data with the aim of better separating the role of the oceans and the biosphere in the global COS budget. . © 2021 Copernicus GmbH. All rights reserved.
语种	英语
scopus关键词	atmospheric chemistry; carbonyl compound; data assimilation; four-dimensional modeling; inverse problem; NOAA satellite; optimization; satellite data
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/247081
作者单位	Institute for Marine and Atmospheric Research, Utrecht University, Utrecht, Netherlands; Meteorology and Air Quality, Wageningen University and Research, Wageningen, Netherlands; Noaa Global Monitoring Laboratory, National Oceanic and Atmospheric Administration, Boulder, CO, United States; Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, Karlsruhe, Germany; Jet Propulsion Laboratory, California Institute of Technology, Pasadena, CA, United States; Rosenstiel School of Marine and Atmospheric Science, University of Miami, Miami, FL, United States
推荐引用方式 GB/T 7714	Ma J.,Kooijmans L.M.J.,Cho A.,et al. Inverse modelling of carbonyl sulfide: Implementation, evaluation and implications for the global budget[J],2021,21(5).
APA	Ma J..,Kooijmans L.M.J..,Cho A..,Montzka S.A..,Glatthor N..,...&Krol M.C..(2021).Inverse modelling of carbonyl sulfide: Implementation, evaluation and implications for the global budget.ATMOSPHERIC CHEMISTRY AND PHYSICS,21(5).
MLA	Ma J.,et al."Inverse modelling of carbonyl sulfide: Implementation, evaluation and implications for the global budget".ATMOSPHERIC CHEMISTRY AND PHYSICS 21.5(2021).