We present here a dynamical method for modelling temporal and geographical variations in ammonia emissions in regional-scale chemistry transport models (CTMs) and chemistry climate models (CCMs). The ...method is based on the meteorology in the models and gridded inventories. We use the dynamical method to investigate the spatiotemporal variability of ammonia emissions across part of Europe and study how these emissions are related to geographical and year-to-year variations in atmospheric temperature alone. For simplicity we focus on the emission from a storage facility related to a standard Danish pig stable with 1000 animals and display how emissions from this source would vary geographically throughout central and northern Europe and from year to year. In view of future climate changes, we also evaluate the potential future changes in emission by including temperature projections from an ensemble of climate models. The results point towards four overall issues. (1) Emissions can easily vary by 20% for different geographical locations within a country due to overall variations in climate. The largest uncertainties are seen for large countries such as the UK, Germany and France. (2) Annual variations in overall climate can at specific locations cause uncertainties in the range of 20%. (3) Climate change may increase emissions by 0-40% in central to northern Europe. (4) Gradients in existing emission inventories that are seen between neighbour countries (e.g. between the UK and France) can be reduced by using a dynamical methodology for calculating emissions. Acting together these four factors can cause substantial uncertainties in emission. Emissions are generally considered among the largest uncertainties in the model calculations made with CTM and CCM models. Efforts to reduce uncertainties are therefore highly relevant. It is therefore recommended that both CCMs and CTMs implement a dynamical methodology for simulating ammonia emissions in a similar way as for biogenic volatile organic compound (BVOCs) - a method that has been used for more than a decade in CTMs. Finally, the climate penalty on ammonia emissions should be taken into account at the policy level such as the NEC and IPPC directives.
The impact of climate change on surface ozone over Europe was studied using four offline regional chemistry transport models (CTMs) and one online regional integrated climate-chemistry model (CCM), ...driven by the same global projection of future climate under the SRES A1B scenario. Anthropogenic emissions of ozone precursors from RCP4.5 for year 2000 were used for simulations of both present and future periods in order to isolate the impact of climate change and to assess the robustness of the results across the different models. The sensitivity of the simulated surface ozone to changes in climate between the periods 2000–2009 and 2040–2049 differs by a factor of two between the models, but the general pattern of change with an increase in southern Europe is similar across different models. Emissions of isoprene differ substantially between different CTMs ranging from 1.6 to 8.0 Tg yr−1 for the current climate, partly due to differences in horizontal resolution of meteorological input data. Also the simulated change in total isoprene emissions varies substantially across models explaining part of the different climate response on surface ozone. Ensemble mean changes in summer mean ozone and mean of daily maximum ozone are close to 1 ppb(v) in parts of the land area in southern Europe. Corresponding changes of 95-percentiles of hourly ozone are close to 2 ppb(v) in the same region. In northern Europe ensemble mean for mean and daily maximum show negative changes while there are no negative changes for the higher percentiles indicating that climate impacts on O3 could be especially important in connection with extreme summer events.
Atmospheric new particle formation (NPF) and growth significantly influences the indirect aerosol-cloud effect within the polar climate system. In this work, the aerosol population is categorised via ...cluster analysis of aerosol number size distributions (9-915 nm, 65 bins) taken at Villum Research Station, Station Nord (VRS) in North Greenland during a 7 year record (2010-2016). Data are clustered at daily averaged resolution; in total, we classified six categories, five of which clearly describe the ultrafine aerosol population, one of which is linked to nucleation events (up to 39% during summer). Air mass trajectory analyses tie these frequent nucleation events to biogenic precursors released by open water and melting sea ice regions. NPF events in the studied regions seem not to be related to bird colonies from coastal zones. Our results show a negative correlation (r = -0.89) between NPF events and sea ice extent, suggesting the impact of ultrafine Arctic aerosols is likely to increase in the future, given the likely increased sea ice melting. Understanding the composition and the sources of Arctic aerosols requires further integrated studies with joint multi-component ocean-atmosphere observation and modelling.
The Danish Eulerian Hemispheric Model (DEHM) is a 3D long-range atmospheric chemistry-transport model with a horizontal domain covering the Northern Hemisphere. For the AQMEII (Air Quality Modelling ...Evaluation International Initiative) inter-comparison exercise, the model was set up with two two-way nested domains simultaneously – one covering Europe and one covering North America. In this paper, the model configuration used in AQMEII will be described, including a discussion of model results and evaluation for the year 2006 against available measurements in Europe for different chemical species. The evaluation of DEHM for Europe shows that the model gives satisfying results for species such as ozone, nitrogen-dioxide, sulphur-dioxide and secondary inorganic aerosols. The evaluation also points to certain processes where DEHM can be improved, such as biogenic emissions of isoprene, mass closure for particulate matter, wet deposition, and description of vertical mixing during winter. Furthermore, special attention is given to the intercontinental transport of air pollution between North America (NA) and Europe (EU). We estimate the contributions to the total air pollution levels at continental scale from the anthropogenic emissions in the two areas, with a focus on ozone and particulate matter using a tagging method, taking into account the non-linear effects of atmospheric chemistry. We conclude that for this specific year, the intercontinental transport between NA and EU is small for the annual or seasonal mean values – for ozone the contributions are typically around 3% (∼1 ppb) from NA to EU and around 1% (∼0.3 ppb) from EU to NA. For particles the contributions from NA to EU is around 0.9% (∼0.05 μg m−3) and from EU to NA around 1.4% (∼0.05 μg m−3).
► We model the air pollution in North America and Europe for the year 2006 using DEHM. ► We evaluate the model results against measurements for Europe for all available species. ► The evaluation leads to conclusions on where to improve the model. ► We calculated the intercontinental transport of air pollution between North America and Europe. ► We found that the exchange of air pollution between the two continents is small on the annual basis.
We examine here the hypothesis that during flowering, the grass pollen concentrations at a specific site reflect the distribution of grass pollen sources within a few kilometres of this site. We ...perform this analysis on data from a measurement campaign in the city of Aarhus (Denmark) using three pollen traps and by comparing these observations with a novel inventory of grass pollen sources. The source inventory is based on a new methodology developed for urban-scale grass pollen sources. The new methodology is believed to be generally applicable for the European area, as it relies on commonly available remote sensing data combined with management information for local grass areas. The inventory has identified a number of grass pollen source areas present within the city domain. The comparison of the measured pollen concentrations with the inventory shows that the atmospheric concentrations of grass pollen in the urban zone reflect the source areas identified in the inventory, and that the pollen sources that are found to affect the pollen levels are located near or within the city domain. The results also show that during days with peak levels of pollen concentrations there is no correlation between the three urban traps and an operational trap located just 60 km away. This finding suggests that during intense flowering, the grass pollen concentration mirrors the local source distribution and is thus a local-scale phenomenon. Model simulations aimed at assessing population exposure to pollen levels are therefore recommended to take into account both local sources and local atmospheric transport, and not to rely only on describing regional to long-range transport of pollen. The derived pollen source inventory can be entered into local-scale atmospheric transport models in combination with other components that simulate pollen release in order to calculate urban-scale variations in the grass pollen load. The gridded inventory with a resolution of 14 m is therefore made available as supplementary material to this paper, and the verifying grass pollen observations are additionally available in tabular form.
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.
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.
The goal of the Tropospheric Ozone Assessment Report (TOAR) is to provide the research community with an up-to-date scientific assessment of tropospheric ozone, from the surface to the tropopause. ...While a suite of observations provides significant information on the spatial and temporal distribution of tropospheric ozone, observational gaps make it necessary to use global atmospheric chemistry models to synthesize our understanding of the processes and variables that control tropospheric ozone abundance and its variability. Models facilitate the interpretation of the observations and allow us to make projections of future tropospheric ozone and trace gas distributions for different anthropogenic or natural perturbations. This paper assesses the skill of current-generation global atmospheric chemistry models in simulating the observed present-day tropospheric ozone distribution, variability, and trends. Drawing upon the results of recent international multi-model intercomparisons and using a range of model evaluation techniques, we demonstrate that global chemistry models are broadly skillful in capturing the spatio-temporal variations of tropospheric ozone over the seasonal cycle, for extreme pollution episodes, and changes over interannual to decadal periods. However, models are consistently biased high in the northern hemisphere and biased low in the southern hemisphere, throughout the depth of the troposphere, and are unable to replicate particular metrics that define the longer term trends in tropospheric ozone as derived from some background sites. When the models compare unfavorably against observations, we discuss the potential causes of model biases and propose directions for future developments, including improved evaluations that may be able to better diagnose the root cause of the model-observation disparity. Overall, model results should be approached critically, including determining whether the model performance is acceptable for the problem being addressed, whether biases can be tolerated or corrected, whether the model is appropriately constituted, and whether there is a way to satisfactorily quantify the uncertainty.
Inverse modeling techniques used to quantify surface carbon fluxes commonly assume that the uncertainty of fossil fuel CO2 (FFCO2 ) emissions is negligible and that intra-annual variations can be ...neglected. To investigate these assumptions, we analyzed the differences between four fossil fuel emission inventories with spatial and temporal differences over Europe and their impact on the model simulated CO2 concentration. Large temporal flux variations characterize the hourly fields (~40 % and ~80 % for the seasonal and diurnal cycles, peak-to-peak) and annual country totals differ by 10 % on average and up to 40 % for some countries (i.e., the Netherlands). These emissions have been prescribed to seven different transport models, resulting in 28 different FFCO2 concentrations fields. The modeled FFCO2 concentration time series at surface sites using time-varying emissions show larger seasonal cycles (+2 ppm at the Hungarian tall tower (HUN)) and smaller diurnal cycles in summer (-1 ppm at HUN) than when using constant emissions. The concentration range spanned by all simulations varies between stations, and is generally larger in winter (up to ~10 ppm peak-to-peak at HUN) than in summer (~5 ppm). The contribution of transport model differences to the simulated concentration std-dev is 2-3 times larger than the contribution of emission differences only, at typical European sites used in global inversions. These contributions to the hourly (monthly) std-dev's amount to ~1.2 (0.8) ppm and ~0.4 (0.3) ppm for transport and emissions, respectively. First comparisons of the modeled concentrations with 14 C-based fossil fuel CO2 observations show that the large transport differences still hamper a quantitative evaluation/validation of the emission inventories. Changes in the estimated monthly biosphere flux (Fbio) over Europe, using two inverse modeling approaches, are relatively small (less that 5 %) while changes in annual Fbio (up to ~0.15 % GtC yr-1 ) are only slightly smaller than the differences in annual emission totals and around 30 % of the mean European ecosystem carbon sink. These results point to an urgent need to improve not only the transport models but also the assumed spatial and temporal distribution of fossil fuel emission inventories.
A local-scale Gaussian dispersion-deposition model (OML-DEP) has been coupled to a regional chemistry-transport model (DEHM with a resolution of approximately 6 km × 6 km over Denmark) in the Danish ...Ammonia Modelling System, DAMOS. Thereby, it has been possible to model the distribution of ammonia concentrations and depositions on a spatial resolution down to 400 m × 400 m for selected areas in Denmark. DAMOS has been validated against measured concentrations from the dense measuring network covering Denmark. Here measured data from 21 sites are included and the validation period covers 2–5 years within the period 2005–2009. A standard time series analysis (using statistic parameters like correlation and bias) shows that the coupled model system captures the measured time series better than the regional- scale model alone. However, our study also shows that about 50% of the modelled concentration level at a given location originates from non-local emission sources. The local-scale model covers a domain of 16 km × 16 km, and of the locally released ammonia (NH3) within this domain, our simulations at five sites show that 14–27% of the locally (within 16 km × 16 km) emitted NH3 also deposits locally. These results underline the importance of including both high-resolution local-scale modelling of NH3 as well as the regional-scale component described by the regional model. The DAMOS system can be used as a tool in environmental management in relation to assessments of total nitrogen load of sensitive nature areas in intense agricultural regions. However, high spatio-temporal resolution in input parameters like NH3 emissions and land-use data is required.
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