Abstract. Aerosols have important impacts on air quality and climate, but the processes affecting their removal from the atmosphere are not fully understood and are poorly constrained by observations. This makes modelled aerosol lifetimes uncertain. In this study, we make use of an observational constraint on aerosol lifetimes provided by radionuclide measurements and investigate the causes of differences within a set of global models. During the Fukushima Dai-Ichi nuclear power plant accident of March 2011, the radioactive isotopes cesium-137 (137Cs) and xenon-133 (133Xe) were released in large quantities. Cesium attached to particles in the ambient air, approximately according to their available aerosol surface area. 137Cs size distribution measurements taken close to the power plant suggested that accumulation-mode (AM) sulfate aerosols were the main carriers of cesium. Hence, 137Cs can be used as a proxy tracer for the AM sulfate aerosol's fate in the atmosphere. In contrast, the noble gas 133Xe behaves almost like a passive transport tracer. Global surface measurements of the two radioactive isotopes taken over several months after the release allow the derivation of a lifetime of the carrier aerosol. We compare this to the lifetimes simulated by 19 different atmospheric transport models initialized with identical emissions of 137Cs that were assigned to an aerosol tracer with each model's default properties of AM sulfate, and 133Xe emissions that were assigned to a passive tracer. We investigate to what extent the modelled sulfate tracer can reproduce the measurements, especially with respect to the observed loss of aerosol mass with time. Modelled 137Cs and 133Xe concentrations sampled at the same location and times as station measurements allow a direct comparison between measured and modelled aerosol lifetime. The e-folding lifetime τe, calculated from station measurement data taken between 2 and 9 weeks after the start of the emissions, is 14.3 days (95 % confidence interval 13.1–15.7 days). The equivalent modelled τe lifetimes have a large spread, varying between 4.8 and 26.7 days with a model median of 9.4 ± 2.3 days, indicating too fast a removal in most models. Because sufficient measurement data were only available from about 2 weeks after the release, the estimated lifetimes apply to aerosols that have undergone long-range transport, i.e. not for freshly emitted aerosol. However, modelled instantaneous lifetimes show that the initial removal in the first 2 weeks was quicker (lifetimes between 1 and 5 days) due to the emissions occurring at low altitudes and co-location of the fresh plume with strong precipitation. Deviations between measured and modelled aerosol lifetimes are largest for the northernmost stations and at later time periods, suggesting that models do not transport enough of the aerosol towards the Arctic. The models underestimate passive tracer (133Xe) concentrations in the Arctic as well but to a smaller extent than for the aerosol (137Cs) tracer. This indicates that in addition to too fast an aerosol removal in the models, errors in simulated atmospheric transport towards the Arctic in most models also contribute to the underestimation of the Arctic aerosol concentrations.

Abstract. A description of the new air quality downscaling model – the urban EMEP (uEMEP) and its combination with the EMEP MSC-W model (European Monitoring and Evaluation Programme Meteorological Synthesising Centre West) – is presented. uEMEP is based on well-known Gaussian modelling principles. The uniqueness of the system is in its combination with the EMEP MSC-W model and the “local fraction” calculation contained within it. This allows the uEMEP model to be imbedded in the EMEP MSC-W model and downscaling can be carried out anywhere within the EMEP model domain, without any double counting of emissions, if appropriate proxy data are available that describe the spatial distribution of the emissions. This makes the model suitable for high-resolution calculations, down to 50 m, over entire countries. An example application, the Norwegian air quality forecasting and assessment system, is described where the entire country is modelled at a resolution of between 250 and 50 m. The model is validated against all available monitoring data, including traffic sites, in Norway. The results of the validation show good results for NO2, which has the best known emissions, and moderately good for PM10 and PM2.5. In Norway, the largest contributor to PM, even in cities, is long-range transport followed by road dust and domestic heating emissions. These contributors to PM are more difficult to quantify than NOx exhaust emission from traffic, which is the major contributor to NO2 concentrations. In addition to the validation results, a number of verification and sensitivity results are summarised. One verification showed that single annual mean calculations with a rotationally symmetric dispersion kernel give very similar results to the average of an entire year of hourly calculations, reducing the runtime for annual means by 4 orders of magnitude. The uEMEP model, in combination with EMEP MSC-W model, provides a new tool for assessing local-scale concentrations and exposure over large regions in a consistent and homogenous way and is suitable for large-scale policy applications.

Now at Statens Forurensningstilsyn, Slrømsveien 96 Oslo, NorwayIn recent decades land-based emissions of air pollutants have been substantially reduced over Europe. At the same time emissions from shipping have continued to grow globally. Emissions from international shipping in sea areas surrounding Europe now contribute about 30% of the EU27 emissions of sulphur and NO x and affect ozone levels all over Europe. Although ozone levels are expected to decrease in most parts of Europe, prognoses for 2020 levels are still above what is considered as threshold values. A growing portion of these impacts can be attributed to emissions from international shipping.This paper presents an evaluation of the impacts on ozone levels in the European mainland due to emissions from international shipping. Calculations are carried out under recent (2004) conditions and for a scenario in 2020, where further emission reductions are applied to land based emissions while the ships emissions increase according to their expected growth in transport volumes, without additional technical reduction measures. Impacts are considered with respect to the formation of ground-level ozone, presented as somo35. We investigate the effect of different shipping emission sources, in particular, international shipping inside the 12 mile zone from the coast, emissions from ships outside the 12 mile zone with EU flags and emissions from ships under other flags. It is shown that contributions from EU ships and non-EU and ships outside the 12 mile zone are about equal in magnitude. Corrected for source strength, the largest effect relative to source strength is from emissions within the 12 mile zone. Here ozone titration may cause reductions in somo35 of more than 10% in some countries, or increases of 5% or more elsewhere.

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