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000013480 1001_ $$0P:(DE-Juel1)VDB1438$$aSchmitgen, S.$$b0$$eCorresponding author$$uFZJ
000013480 245__ $$aUse of airborne CO measurements for Lagrangian of ozone formation and transport in continental plumes
000013480 260__ $$aJülich$$bForschungszentrum,  Zentralbibliothek$$c2001
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000013480 520__ $$aThe anthropogenic ozone budget is investigated in remote regions with respect to the influence of emissions of VOC and NO., at source regions, and with regard to the relative roles of ozone formation in the polluted boundary layer (PBL) and in the free troposphere (FT). The investigation makes use of airborne measurements aboard the United Kingdom Meteorological Office (UKMO) C-130 Hercules aircraft obtained during the European project TACIA (Testing Atmospheric Chemistry in Anticyclones) and the UK project ACSOE (Atmospheric Chemistry Studies in Oceanic Environment). High resolution measurements ofCO as a quasi-inert tracer of anthropogenic emissions were made and interpreted . The experimental investigations of anthropogenic plumes in the planetary boundary layer (TACIA) and the remote free troposphere (ACSOE) are interpreted by heuristic model calculations . The model set-up, with modules for transport and chemistry, allows for a separation of these processes in the analysis. The transport module in combination with the CO observations is shown to be a useful tool for the analysis of emissions and transport . Convective transport into the free troposphere is identified by combination of the transport module with satellite data. The interpretation of observations distant from the source regions, with respect to the influence of anthropogenic VOC and NO, emissions on the ozone formation in a plume, is made by an indirect inverse modelling approach. The method involves extensive sensitivity studies regarding various initial VOC and NO,, concentrations, in an EKMA framework. Despite the large degree of abstraction, the results of EKMA plot calculations can be compared to the measurements with the help ofCO as emission tracer and enable the dependency of the observed 03 on anthropogenic VOC and NO,, emissions to be analysed. A central point of this study is the use of statistical test methods for the analysis of the significance of deviations between model results and measurements . Sensitivity studies, regarding the dependence of model results on the variability of input parameters, are analysed with respect to confidence regions of the observations . With these means, the following general conclusions regarding ozone formation in continental plumes transported into source free maritime areas are obtained: The layers of enhanced CO and 03 in the FT, observed during ACSOE flight A575, can only partly be explained by in-situ production of ozone in the FT. Higher 03 production efficiencies on a per-molecule basis of NO,, in the FT compared to the PBL are found to be compensated by the reduced NO, availability in the free troposphere, related to CO. PBL-produced 03 is found not only to be important close to source regions, but also for long range transport within the FT in connection with cloud venting, where it contributes to the tropospherc budget of ozone. The 03 formation within the PBL depends on a multitude of parameters. It is shown for the example of the TACIA flight A581, that the natural variability and uncertainties of these parameters are still too high for an unambiguous interpretation of observed 03 formation in a continental plume with respect to anthropogenic NQ, and VOC emissions. This complicates the task of estimating the influence of export of pollutionderived ozone and its precursors on the remote troposphere .
000013480 536__ $$0G:(DE-Juel1)FUEK72$$2G:(DE-HGF)$$aChemie der Belasteten Atmosphäre$$c36.20.0$$x0
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