| DOI: | 10.1002/2015GL063102
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| 论文题名: | Clumped isotope perturbation in tropospheric nitrous oxide from stratospheric photolysis |
| 作者: | Schmidt J.A.; Johnson M.S.
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| 刊名: | Geophysical Research Letters
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| ISSN: | 0094-8708
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| EISSN: | 1944-8439
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| 出版年: | 2015
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| 卷: | 42, 期:9 | | 起始页码: | 3546
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| 结束页码: | 3552
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| 语种: | 英语
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| 英文关键词: | clumped isotopes
; isotopomer
; nitrogen cycle
; nitrous oxide
; quantum chemistry
; stratosphere
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| Scopus关键词: | Budget control
; Greenhouse gases
; Isotopes
; Mass spectrometry
; Nitrogen oxides
; Quantum chemistry
; Quantum theory
; Troposphere
; Upper atmosphere
; Accurate measurement
; Clumped isotopes
; Isotopic composition
; Isotopomer
; Nitrogen cycles
; Nitrous oxide
; Time-dependent quantum dynamics
; Ultraviolet absorption
; Photolysis
; atmospheric modeling
; isotopic composition
; nitrous oxide
; photochemistry
; photolysis
; quantum mechanics
; stratosphere
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| 英文摘要: | Nitrous oxide (N2O) is potent greenhouse gas and source of ozone depleting NO to the stratosphere. Recent advances in mass spectrometry allow accurate measurement of multiply substituted ("clumped") N2O isotopocules, providing new constraints on the N2O source budget. However, this requires a quantification of the "clumped" N2O fractionation from stratospheric photolysis (main sink). We use time-dependent quantum dynamics and a 1-D atmospheric model to determine the effect of stratospheric photolysis on the abundances of multisubstituted N2O isotopocules in the atmosphere. The ultraviolet absorption cross sections of 557 (i.e., 15N15N17O), 458, 548, 457, and 547 are presented for the first time and used to derive altitude-dependent photolysis rates and fractionation constants. We find that photolysis alters the N2O isotopic composition with multisubstituted mass 47 isotopocules being less abundant than expected from stochastics (Δ47=-1.7‰ in the troposphere and down to -12‰ in the upper stratosphere). Key Points Stratospheric photochemistry will have a large impact on tropospheric N2O This is the first determination of the N2O isotopocule cross sections Multiple isotopes are the key to reducing uncertainties in N2O emissions budget ©2015. American Geophysical Union. All Rights Reserved. |
| URL: | https://www.scopus.com/inward/record.uri?eid=2-s2.0-84930475558&doi=10.1002%2f2015GL063102&partnerID=40&md5=35dc1c92ab9c2136b921d8ea29580c70
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| Citation statistics: |
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| 资源类型: | 期刊论文
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| 标识符: | http://119.78.100.158/handle/2HF3EXSE/8324
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| Appears in Collections: | 科学计划与规划
气候变化与战略
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作者单位: | Department of Chemistry, University of Copenhagen, Copenhagen, Denmark
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| Recommended Citation: | |
Schmidt J.A.,Johnson M.S.. Clumped isotope perturbation in tropospheric nitrous oxide from stratospheric photolysis[J]. Geophysical Research Letters,2015-01-01,42(9).
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