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DOI10.5194/acp-21-11113-2021
Impact of stratospheric air and surface emissions on tropospheric nitrous oxide during ATom
Gonzalez Y.; Commane R.; Manninen E.; Daube B.C.; Schiferl L.D.; McManus J.B.; McKain K.; Hintsa E.J.; Elkins J.W.; Montzka S.A.; Sweeney C.; Moore F.; Jimenez J.L.; Campuzano Jost P.; Ryerson T.B.; Bourgeois I.; Peischl J.; Thompson C.R.; Ray E.; Wennberg P.O.; Crounse J.; Kim M.; Allen H.M.; Newman P.A.; Stephens B.B.; Apel E.C.; Hornbrook R.S.; Nault B.A.; Morgan E.; Wofsy S.C.
发表日期2021
ISSN1680-7316
起始页码11113
结束页码11132
卷号21期号:14
英文摘要We measured the global distribution of tropospheric N2O mixing ratios during the NASA airborne Atmospheric Tomography (ATom) mission. ATom measured concentrations of g1/4g300 gas species and aerosol properties in 647 vertical profiles spanning the Pacific, Atlantic, Arctic, and much of the Southern Ocean basins, nearly from pole to pole, over four seasons (2016-2018). We measured N2O concentrations at 1gHz using a quantum cascade laser spectrometer (QCLS). We introduced a new spectral retrieval method to account for the pressure and temperature sensitivity of the instrument when deployed on aircraft. This retrieval strategy improved the precision of our ATom QCLS N2O measurements by a factor of three (based on the standard deviation of calibration measurements). Our measurements show that most of the variance of N2O mixing ratios in the troposphere is driven by the influence of N2O-depleted stratospheric air, especially at mid- and high latitudes. We observe the downward propagation of lower N2O mixing ratios (compared to surface stations) that tracks the influence of stratosphere-troposphere exchange through the tropospheric column down to the surface. The highest N2O mixing ratios occur close to the Equator, extending through the boundary layer and free troposphere. We observed influences from a complex and diverse mixture of N2O sources, with emission source types identified using the rich suite of chemical species measured on ATom and the geographical origin calculated using an atmospheric transport model. Although ATom flights were mostly over the oceans, the most prominent N2O enhancements were associated with anthropogenic emissions, including from industry (e.g., oil and gas), urban sources, and biomass burning, especially in the tropical Atlantic outflow from Africa. Enhanced N2O mixing ratios are mostly associated with pollution-related tracers arriving from the coastal area of Nigeria. Peaks of N2O are often associated with indicators of photochemical processing, suggesting possible unexpected source processes. In most cases, the results show how difficult it is to separate the mixture of different sources in the atmosphere, which may contribute to uncertainties in the N2O global budget. The extensive data set from ATom will help improve the understanding of N2O emission processes and their representation in global models. © 2021 Yenny Gonzalez et al.
语种英语
scopus关键词atmospheric chemistry; biomass burning; concentration (composition); nitrous oxide; sensitivity analysis; source apportionment; stratosphere; tracer; troposphere; Nigeria
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/246710
作者单位John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138, United States; Cimel Electronique, Paris, 75011, France; Izaña Atmospheric Research Centre, Santa Cruz de Tenerife, 38001, Spain; Dept. of Earth and Environmental Science, Columbia University, New York, NY 10027, United States; Lamont-Doherty Earth Observatory, Columbia University, Palisades, NY 10964, United States; Center for Atmospheric and Environmental Chemistry, Aerodyne Research Inc., Billerica, MA 01821, United States; Noaa Global Monitoring Laboratory, Boulder, CO 80305, United States; Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado Boulder, Boulder, CO 80309, United States; Noaa Chemical Sciences Laboratory, Boulder, CO 80305, United States; Division of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA 91125, United States; Division of Engineering and Applied Science, California Institute of Technology, Pasaden...
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Gonzalez Y.,Commane R.,Manninen E.,et al. Impact of stratospheric air and surface emissions on tropospheric nitrous oxide during ATom[J],2021,21(14).
APA Gonzalez Y..,Commane R..,Manninen E..,Daube B.C..,Schiferl L.D..,...&Wofsy S.C..(2021).Impact of stratospheric air and surface emissions on tropospheric nitrous oxide during ATom.ATMOSPHERIC CHEMISTRY AND PHYSICS,21(14).
MLA Gonzalez Y.,et al."Impact of stratospheric air and surface emissions on tropospheric nitrous oxide during ATom".ATMOSPHERIC CHEMISTRY AND PHYSICS 21.14(2021).
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