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Empa, Swiss Federal Laboratories for Materials Science and Technology,
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A Kalman-filter based inverse emission estimation method for long-lived trace gases is presented for use in conjunction with a Lagrangian particle dispersion model like FLEXPART. The sequential nature of the approach allows tracing slow seasonal and interannual changes rather than estimating a single period-mean emission field. Other important features include the estimation of a slowly varying concentration background at each measurement station, the possibility to constrain the solution to non-negative emissions, the quantification of uncertainties, the consideration of temporal correlations in the residuals, and the applicability to potentially large inversion problems. The method is first demonstrated for a set of synthetic observations created from a prescribed emission field with different levels of (correlated) noise, which closely mimics true observations. It is then applied to real observations of the three halocarbons HFC-125, HFC-152a and HCFC-141b at the remote research stations Jungfraujoch and Mace Head for the quantification of emissions in Western European countries from 2006 to 2010. Estimated HFC-125 emissions are mostly consistent with national totals reported to the Kyoto protocol and show a generally increasing trend over the considered period. Results for HFC-152a are much more variable with estimated emissions being both higher and lower in different countries. The highest emissions of the order of 1000 Mg yr-1 are estimated for Italy which so far does not report HFC-152a emissions. Emissions of HCFC-141b show a continuing strong decrease as expected due to its ban under the Montreal Protocol. Emissions from France, however, were still rather large (near 1000 Mg yr-1) in the years 2006 and 2007 but strongly declined thereafter.
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Ground-based in situ measurements of hydrofluorocarbons HFC-125, HFC-134a, and HFC-152a, which are regulated under the Kyoto Protocol, are carried out at four European sites within the SOGE (System of Observation of Halogenated Greenhouse Gases in Europe) program. Concentrations measured at the high mountain stations of Jungfraujoch (Switzerland) and Mte Cimone (Italy) together with back-trajectory statistical analysis are used in order to identify potential source regions on a European scale. Combining concentration data recorded at the two sites allows to reduce one of the problem which is inherent to the back-trajectory approach, i.e. the localisation of "ghost" sources in the wake of real sources. In this way, a more reliable picture of the location of European potential source regions is given.