Abstract. The CO 2 source and sink distribution across Europe can be estimated in principle through inverse methods by combining CO 2 observations and atmospheric transport models. Uncertainties of such estimates are mainly due to insufficient spatiotemporal coverage of CO 2 observations and biases of the models. In order to assess the biases related to the use of different models the CO 2 concentration field over Europe has been simulated with five different Eulerian atmospheric transport models as part of the EU-funded AE-ROCARB project, which has the main goal to estimate the carbon balance of Europe. In contrast to previous comparisons, here both global coarse-resolution and regional higherresolution models are included. Continuous CO 2 observations from continental, coastal and mountain sites as well as flasks sampled on aircrafts are used to evaluate the models' ability to capture the spatiotemporal variability and distribution of lower troposphere CO 2 across Europe. 14 CO 2 is used in addition to evaluate separately fossil fuel signal predictions. The simulated concentrations show a large range of variation, with up to ∼10 ppm higher surface concentrations over Western and Central Europe in the regional models with highest (mesoscale) spatial resolution.The simulation -data comparison reveals that generally high-resolution models are more successful than coarse models in capturing the amplitude and phasing of the observed Correspondence to: C. Geels (cag@dmu.dk) short-term variability. At high-altitude stations the magnitude of the differences between observations and models and in between models is less pronounced, but the timing of the diurnal cycle is not well captured by the models.The data comparisons show also that the timing of the observed variability on hourly to daily time scales at lowaltitude stations is generally well captured by all models. However, the amplitude of the variability tends to be underestimated. While daytime values are quite well predicted, nighttime values are generally underpredicted. This is a reflection of the different mixing regimes during day and night combined with different vertical resolution between models. In line with this finding, the agreement among models is increased when sampling in the afternoon hours only and when sampling the mixed portion of the PBL, which amounts to sampling at a few hundred meters above ground. The main recommendations resulting from the study for constraining land carbon sources and sinks using high-resolution concentration data and state-of-the art transport models through inverse methods are given in the following: 1) Low altitude stations are presently preferable in inverse studies. If high altitude stations are used then the model level that represents the specific sites should be applied, 2) at low altitude sites only the afternoon values of concentrations can be represented sufficiently well by current models and therefore afternoon values are more appropriate for constraining large-scale sources and sinks in combination with tr...

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Deriving a parameterisation of ammonia emissions for use in chemistry-transport models (CTMs) is a complex problem as the emission varies locally as a result of local climate and local agricultural management. In current CTMs such factors are generally not taken into account. This paper demonstrates how local climate and local management can be accounted for in CTMs by applying a modular approach for deriving data as input to a dynamic ammonia emission model for Europe. Default data are obtained from information in the RAINS system, and it is demonstrated how this dynamic emission model based on these input data improves the NH₃ calculations in a CTM model when the results are compared with calculations obtained by traditional methods in emission handling. It is also shown how input data can be modified over a specific target region resulting in even further improvement in performance over this domain. The model code and the obtained default values for the modelling experiments are available as supplementary information to this article for use by the modelling community on similar terms as the EMEP CTM model: the GPL licencse v3

Abstract. We have developed an integrated model system, EVA (Economic Valuation of Air pollution), based on the impact-pathway chain, to assess the health-related economic externalities of air pollution resulting from specific emission sources or sectors, which can be used to support policy-making with respect to emission control. Central for the system is a newly developed tagging method capable of calculating the contribution from a specific emission source or sector to the overall air pollution levels, taking into account the non-linear atmospheric chemistry. The main objective of this work is to identify the anthropogenic emission sources in Europe and Denmark that contribute the most to human health impacts. In this study, we applied the EVA system to Europe and Denmark, with a detailed analysis of health-related external costs from the ten major emission sectors and their relative contributions. The paper contains a thorough description of the EVA system, the main results from the assessment of the main contributors and a discussion of the most important atmospheric chemical reactions relevant for interpreting the results. The main conclusion from the analysis is that the major contributors to health-related external costs are major power production, agriculture, road traffic, and non-industrial domestic combustion, including wood combustion. We conclude that when regulating the emissions of ammonia from the agricultural sector, both the impacts on nature and on human health should be taken into account. This study confirms that air pollution constitutes a serious problem for human health and that the related external costs are considerable. The results in this work emphasize the importance of defining the right questions in the decision-making process. The results from assessing the impacts from each emission sector depend clearly on the assumption that the other emission sectors are not changed, especially emissions changing concentrations of atmospheric OH and therefore lifetimes of other chemical species.

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Abstract.A new 3-D mercury model has been developed within the Danish Arctic Monitoring and Assessment Programme (AMAP). The model is based on the Danish Eulerian Hemispheric Model, which in the original version has been used to study the transport of SO 2 , SO 2− 4 and Pb into the Arctic. It was developed for sulphur in 1990 and in 1999 also lead was included. For the current study a chemical scheme for mercury has been included and the model is now applied to the mercury transport problem. Some experiments with the formulation of the mercury chemistry during the Polar Sunrise are carried out in order to investigate the observed depletion. Some of the main conclusions of the work described in this paper are that atmospheric transport of mercury is a very important pathway into the Arctic and that mercury depletion in the Arctic troposphere during the Polar Sunrise contributes considerably to the deposition of mercury in the Arctic.

Abstract. A tracer model, DREAM (the Danish Rimpuff andEulerian Accidental release Model), has been developed for modelling transport, dispersion and deposition (wet and dry) of radioactive material from accidental releases, as the Chernobyl accident. The model is a combination of a Lagrangian model, that includes the near source dispersion, and an Eulerian model describing the long-range transport. The performance of the transport model has previously been tested within the European Tracer Experiment, ETEX, which included transport and dispersion of an inert, non-depositing tracer from a controlled release. The focus of this paper is the model performance with respect to the total deposition of 137 Cs, 134 Cs and 131 I from the Chernobyl accident, using different relatively simple and comprehensive parameterizations for dry-and wet deposition. The performance, compared to measurements, of using different combinations of two different wet deposition parameterizations and three different parameterizations of dry deposition has been evaluated, using different statistical tests. The best model performance, compared to measurements, is obtained when parameterizing the total deposition combined of a simple method for dry deposition and a subgrid-scale averaging scheme for wet deposition based on relative humidities. The same major conclusion is obtained for all the three different radioactive isotopes and using two different deposition measurement databases. Large differences are seen in the results obtained by using the two different parameterizations of wet deposition based on precipitation rates and relative humidities, respectively. The parameterization based on subgrid-scale averaging is, in all cases, performing better than the parameterization based on precipitation rates. This indicates that the in-cloud scavenging process is more important than the beCorrespondence to: J. Brandt (jbr@dmu.dk) low cloud scavenging process for the submicron particles and that the precipitation rates are relatively uncertain in the meteorological model compared to the relative humidity. Relatively small differences are, however, seen in the statistical tests between the three different parameterizations of dry deposition.

An integrated model system, EVA (Economic Valuation of Air pollution), based on the impact-pathway chain has been developed to assess the health-related economic externalities of air pollution resulting from specific emission sources or sectors. The model system can be used to support policy-making with respect to emission control. In this study, we apply the EVA system to Europe, and perform a more detailed assessment of past, present, and future health-cost externalities of the total air pollution levels in Europe (including both natural and anthropogenic sources), represented by the years 2000, 2007, 2011, and 2020. We also assess the contribution to the health-related external costs from international ship traffic with special attention to the international ship traffic in the Baltic and North seas, since special regulatory actions on sulfur emissions, called SECA (sulfur emission control area), have been introduced in these areas. We conclude that, despite efficient regulatory actions in Europe in recent decades, air pollution still constitutes a serious problem for human health. Hence the related external costs are considerable. The total health-related external costs for the whole of Europe are estimated at 803 bn euros yr⁻¹ for the year 2000, decreasing to 537 bn euros yr⁻¹ in the year 2020. We estimate the total number of premature deaths in Europe in the year 2000 due to air pollution to be around 680 000 yr⁻¹, decreasing to approximately 450 000 in the year 2020. The contribution from international ship traffic in the Northern Hemisphere was estimated to 7% of the total health-related external costs in Europe in the year 2000, increasing to 12% in the year 2020. In contrast, the contribution from international ship traffic in the Baltic Sea and the North Sea decreases 36% due to the regulatory efforts of reducing sulfur emissions from ship traffic in SECA. Introducing this regulatory instrument for all international ship traffic in the Northern Hemisphere, or at least in areas close to Europe, would have a significant positive impact on human health in Europe