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    | Titel | A model study of the impact of source gas changes on the stratosphere for 1850–2100 |  
    | VerfasserIn | E. L. Fleming, C. H. Jackman, R. S. Stolarski, A. R. Douglass |  
    | Medientyp | Artikel 
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    | Sprache | Englisch 
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    | ISSN | 1680-7316 
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    | Digitales Dokument | URL |  
    | Erschienen | In: Atmospheric Chemistry and Physics ; 11, no. 16 ; Nr. 11, no. 16 (2011-08-22), S.8515-8541 |  
    | Datensatznummer | 250010019 
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    | Publikation (Nr.) |  copernicus.org/acp-11-8515-2011.pdf |  
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        | Zusammenfassung |  
        | The long-term stratospheric impacts due to emissions of
      CO2, CH4, N2O, and ozone depleting
      substances (ODSs) are investigated using an updated version of
      the Goddard two-dimensional (2-D) model. Perturbation
      simulations with the ODSs, CO2, CH4, and
      N2O varied individually are performed to isolate the
      relative roles of these gases in driving stratospheric changes
      over the 1850–2100 time period. We also show comparisons with
      observations and the Goddard Earth Observing System
      chemistry-climate model simulations for the time period
      1960–2100 to illustrate that the 2-D model captures the basic
      processes responsible for long-term stratospheric change. 
 The ODSs, CO2, CH4, and N2O impact ozone via
      several mechanisms. ODS and N2O loading decrease
      stratospheric ozone via the increases in atmospheric halogen and
      odd nitrogen species, respectively. CO2 loading impacts
      ozone by: (1) cooling the stratosphere which increases ozone via
      the reduction in the ozone chemical loss rates, and (2) accelerating the Brewer-Dobson circulation (BDC) which
      redistributes ozone in the lower stratosphere. The net result of
      CO2 loading is an increase in global ozone in the total
      column and upper stratosphere. CH4 loading impacts ozone
      by: (1) increasing atmospheric H2O and the odd hydrogen
      species which decreases ozone via the enhanced HOx-ozone loss
      rates; (2) increasing the H2O cooling of the middle
      atmosphere which reduces the ozone chemical loss rates,
      partially offsetting the enhanced HOx-ozone loss; (3) converting
      active to reservoir chlorine via the reaction
      CH4+Cl→HCl+CH3 which leads to more ozone; and (4) increasing the NOx-ozone production in the
      troposphere. The net result of CH4 loading is an ozone
      decrease above 40–45 km, and an increase below 40–45 km and in
      the total column.
 
 The 2-D simulations indicate that prior to 1940, the ozone
      increases due to CO2 and CH4 loading outpace
      the ozone losses due to increasing N2O and carbon
      tetrachloride (CCl4) emissions, so that total column and
      upper stratospheric global ozone reach broad maxima during the
      1920s–1930s. This precedes the
      significant ozone depletion during ~1960–2050 driven by
      the ODS loading. During the latter half of the 21st century as
      ODS emissions diminish, CO2, N2O, and
      CH4 loading will all have significant impacts on
      global total ozone based on the Intergovernmental Panel on
      Climate Change (IPCC) A1B (medium) scenario,
      with CO2 having the largest individual
      effect. Sensitivity tests illustrate that due to the strong
      chemical interaction between methane and chlorine, the
      CH4 impact on total ozone becomes significantly more
      positive with larger ODS loading. The model simulations also
      show that changes in stratospheric temperature, BDC, and age of
      air during 1850–2100 are
      controlled mainly by the CO2 and ODS loading. The
      simulated acceleration of the BDC causes the global average age of air above 22 km to
      decrease by ~1 yr from 1860–2100. The
      photochemical lifetimes of N2O, CFCl3,
      CF2Cl2, and CCl4 decrease by 11–13 %
      during 1960–2100 due to the acceleration of the BDC, with
      much smaller lifetime changes (<4 %) caused by changes in
      the photochemical loss rates.
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