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.

Halocarbons are powerful greenhouse gases capable of significantly influencing the radiative forcing of the Earth’s atmosphere. Halocarbons are monitored in several stations which are globally distributed in order to assess long term atmospheric trends and to identify source regions. However, to achieve these aims the definition of background mixing ratios, i.e. the mixing ratio in a given air mass when the recent contribution of local sources is absent, is necessary. This task can be accomplished using different methods. This paper presents a statistical methodology that has been devised specifically for a mountain site located in Continental Europe (Monte Cimone, Italy), characterised by the vicinity of strong sources. The method involves the decomposition of the observed data distribution into a Gaussian distribution, representative of background values, and a Gamma distribution, ascribable to contribution from stronger sources. The method has been applied to a time series from a European marine remote station (Mace Head, Ireland) as well as to time series from Monte Cimone. A comparison of the methodology described in this paper with a well-established meteorological filtering procedure at Mace Head has shown an excellent agreement. A comparison of the baselines at Mace Head, Mt. Cimone and the Swiss alpine station of the Jungfraujoch highlighted the occurrence of a specific background concentration. Although this paper presents the application of the method to three hydrofluorocarbons, the proposed methodology can be extended to any long lived atmospheric component for which a long term time series is available and at any location even if affected by strong source regions.

This paper presents an analysis of the recent tropospheric molecular hydrogen (H2) budget with a particular focus on soil uptake and European surface emissions. A variational inversion scheme is combined with observations from the RAMCES and EUROHYDROS atmospheric networks, which include continuous measurements performed between mid-2006 and mid-2009. Net H2 surface flux, then deposition velocity and surface emissions and finally, deposition velocity, biomass burning, anthropogenic and N2 fixation-related emissions were simultaneously inverted in several scenarios. These scenarios have focused on the sensibility of the soil uptake value to different spatio-temporal distributions. The range of variations of these diverse inversion sets generate an estimate of the uncertainty for each term of the H2 budget. The net H2 flux per region (High Northern Hemisphere, Tropics and High Southern Hemisphere) varies between ?8 and +8 Tg yr?1. The best inversion in terms of fit to the observations combines updated prior surface emissions and a soil deposition velocity map that is based on bottom-up and top-down estimations. Our estimate of global H2 soil uptake is ?59±9 Tg yr?1. Forty per cent of this uptake is located in the High Northern Hemisphere and 55% is located in the Tropics. In terms of surface emissions, seasonality is mainly driven by biomass burning emissions. The inferred European anthropogenic emissions are consistent with independent H2 emissions estimated using a H2/CO mass ratio of 0.034 and CO emissions within the range of their respective uncertainties. Additional constraints, such as isotopic measurements would be needed to infer a more robust partition of H2 sources and sinks.