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1.
  • Flechard, Chris R., et al. (author)
  • Carbon-nitrogen interactions in European forests and semi-natural vegetation - Part 1: Fluxes and budgets of carbon, nitrogen and greenhouse gases from ecosystem monitoring and modelling
  • 2020
  • In: Biogeosciences. - : Copernicus GmbH. - 1726-4170 .- 1726-4189. ; 17:6, s. 1583-1620
  • Journal article (peer-reviewed)abstract
    • The impact of atmospheric reactive nitrogen (N-r) deposition on carbon (C) sequestration in soils and biomass of unfertilized, natural, semi-natural and forest ecosystems has been much debated. Many previous results of this dC/dN response were based on changes in carbon stocks from periodical soil and ecosystem inventories, associated with estimates of N-r deposition obtained from large-scale chemical transport models. This study and a companion paper (Flechard et al., 2020) strive to reduce uncertainties of N effects on C sequestration by linking multi-annual gross and net ecosystem productivity estimates from 40 eddy covariance flux towers across Europe to local measurement-based estimates of dry and wet N-r deposition from a dedicated collocated monitoring network. To identify possible ecological drivers and processes affecting the interplay between C and N-r inputs and losses, these data were also combined with in situ flux measurements of NO, N2O and CH4 fluxes; soil NO3- leaching sampling; and results of soil incubation experiments for N and greenhouse gas (GHG) emissions, as well as surveys of available data from online databases and from the literature, together with forest ecosystem (BAS-FOR) modelling. Multi-year averages of net ecosystem productivity (NEP) in forests ranged from -70 to 826 gCm(-2) yr(-1) at total wet + dry inorganic N-r deposition rates (N-dep) of 0.3 to 4.3 gNm(-2) yr(-1) and from -4 to 361 g Cm-2 yr(-1) at N-dep rates of 0.1 to 3.1 gNm(-2) yr(-1) in short semi-natural vegetation (moorlands, wetlands and unfertilized extensively managed grasslands). The GHG budgets of the forests were strongly dominated by CO2 exchange, while CH4 and N2O exchange comprised a larger proportion of the GHG balance in short semi-natural vegetation. Uncertainties in elemental budgets were much larger for nitrogen than carbon, especially at sites with elevated N-dep where N-r leaching losses were also very large, and compounded by the lack of reliable data on organic nitrogen and N-2 losses by denitrification. Nitrogen losses in the form of NO, N2O and especially NO3- were on average 27%(range 6 %-54 %) of N-dep at sites with N-dep < 1 gNm(-2) yr(-1) versus 65% (range 35 %-85 %) for N-dep > 3 gNm(-2) yr(-1). Such large levels of N-r loss likely indicate that different stages of N saturation occurred at a number of sites. The joint analysis of the C and N budgets provided further hints that N saturation could be detected in altered patterns of forest growth. Net ecosystem productivity increased with N-r deposition up to 2-2.5 gNm(-2) yr(-1), with large scatter associated with a wide range in carbon sequestration efficiency (CSE, defined as the NEP/GPP ratio). At elevated N-dep levels (> 2.5 gNm(-2) yr(-1)), where inorganic N-r losses were also increasingly large, NEP levelled off and then decreased. The apparent increase in NEP at low to intermediate N-dep levels was partly the result of geographical cross-correlations between N-dep and climate, indicating that the actual mean dC/dN response at individual sites was significantly lower than would be suggested by a simple, straightforward regression of NEP vs. N-dep.
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2.
  • McFiggans, Gordon, et al. (author)
  • Secondary organic aerosol reduced by mixture of atmospheric vapours
  • 2019
  • In: Nature. - : Springer Science and Business Media LLC. - 0028-0836 .- 1476-4687. ; 565:7741, s. 587-593
  • Journal article (peer-reviewed)abstract
    • Secondary organic aerosol contributes to the atmospheric particle burden with implications for air quality and climate. Biogenic volatile organic compounds such as terpenoids emitted from plants are important secondary organic aerosol precursors with isoprene dominating the emissions of biogenic volatile organic compounds globally. However, the particle mass from isoprene oxidation is generally modest compared to that of other terpenoids. Here we show that isoprene, carbon monoxide and methane can each suppress the instantaneous mass and the overall mass yield derived from monoterpenes in mixtures of atmospheric vapours. We find that isoprene 'scavenges' hydroxyl radicals, preventing their reaction with monoterpenes, and the resulting isoprene peroxy radicals scavenge highly oxygenated monoterpene products. These effects reduce the yield of low-volatility products that would otherwise form secondary organic aerosol. Global model calculations indicate that oxidant and product scavenging can operate effectively in the real atmosphere. Thus highly reactive compounds (such as isoprene) that produce a modest amount of aerosol are not necessarily net producers of secondary organic particle mass and their oxidation in mixtures of atmospheric vapours can suppress both particle number and mass of secondary organic aerosol. We suggest that formation mechanisms of secondary organic aerosol in the atmosphere need to be considered more realistically, accounting for mechanistic interactions between the products of oxidizing precursor molecules (as is recognized to be necessary when modelling ozone production).
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3.
  • Mills, Gina, et al. (author)
  • Evidence of widespread effects of ozone on crops and (semi-)natural vegetation in Europe (1990 - 2006) in relation to AOT40 - and flux-based risk maps
  • 2010
  • In: Global Change Biology. - : Wiley. - 1365-2486 .- 1354-1013. ; 17:1, s. 592-613
  • Journal article (peer-reviewed)abstract
    • Records of effects of ambient ozone pollution on vegetation have been compiled for Europe for the years 1990–2006. Sources include scientific papers, conference proceedings, reports to research funders, records of confirmed ozone injury symptoms and an international biomonitoring experiment coordinated by the ICP Vegetation. The latter involved ozone-sensitive (NC-S) and ozone-resistant (NC-R) biotypes of white clover (Trifolium repens L.) grown according to a common protocol and monitored for ozone injury and biomass differences in 17 European countries, from 1996 to 2006. Effects were separated into visible injury or growth/yield reduction. Of the 644 records of visible injury, 39% were for crops (27 species), 38.1% were for (semi-) natural vegetation (95 species) and 22.9% were for shrubs (49 species). Owing to inconsistencies in reporting effort from year to year it was not possible to determine geographical or temporal trends in the data. Nevertheless, this study has shown effects in ambient air in 18 European countries from Sweden in the north to Greece in the south. These effects data were superimposed on AOT40 (accumulated ozone concentrations over 40 ppb) and POD3gen (modelled accumulated stomatal flux over a threshold of 3 nmol m−2 s−1) maps generated by the EMEP Eulerian model (50 km × 50 km grid) that were parameterized for a generic crop based on wheat and NC-S/NC-R white clover. Many effects were found in areas where the AOT40 (crops) was below the critical level of 3 ppm h. In contrast, the majority of effects were detected in grid squares where POD3gen (crops) were in the mid-high range (>12 mmol m−2). Overall, maps based on POD3gen provided better fit to the effects data than those based on AOT40, with the POD3gen model for clover fitting the clover effects data better than that for a generic crop.
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4.
  • Aas, W., et al. (author)
  • Lessons learnt from the first EMEP intensive measurement periods
  • 2012
  • In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 12:17, s. 8073-8094
  • Journal article (peer-reviewed)abstract
    • The first EMEP intensive measurement periods were held in June 2006 and January 2007. The measurements aimed to characterize the aerosol chemical compositions, including the gas/aerosol partitioning of inorganic compounds. The measurement program during these periods included daily or hourly measurements of the secondary inorganic components, with additional measurements of elemental- and organic carbon (EC and OC) and mineral dust in PM1, PM2.5 and PM10. These measurements have provided extended knowledge regarding the composition of particulate matter and the temporal and spatial variability of PM, as well as an extended database for the assessment of chemical transport models. This paper summarise the first experiences of making use of measurements from the first EMEP intensive measurement periods along with EMEP model results from the updated model version to characterise aerosol composition. We investigated how the PM chemical composition varies between the summer and the winter month and geographically. The observation and model data are in general agreement regarding the main features of PM10 and PM2.5 composition and the relative contribution of different components, though the EMEP model tends to give slightly lower estimates of PM10 and PM2.5 compared to measurements. The intensive measurement data has identified areas where improvements are needed. Hourly concurrent measurements of gaseous and particulate components for the first time facilitated testing of modelled diurnal variability of the gas/aerosol partitioning of nitrogen species. In general, the modelled diurnal cycles of nitrate and ammonium aerosols are in fair agreement with the measurements, but the diurnal variability of ammonia is not well captured. The largest differences between model and observations of aerosol mass are seen in Italy during winter, which to a large extent may be explained by an underestimation of residential wood burning sources. It should be noted that both primary and secondary OC has been included in the calculations for the first time, showing promising results. Mineral dust is important, especially in southern Europe, and the model seems to capture the dust episodes well. The lack of measurements of mineral dust hampers the possibility for model evaluation for this highly uncertain PM component. There are also lessons learnt regarding improved measurements for future intensive periods. There is a need for increased comparability between the measurements at different sites. For the nitrogen compounds it is clear that more measurements using artefact free methods based on continuous measurement methods and/or denuders are needed. For EC/OC, a reference methodology (both in field and laboratory) was lacking during these periods giving problems with comparability, though measurement protocols have recently been established and these should be followed by the Parties to the EMEP Protocol. For measurements with no defined protocols, it might be a good solution to use centralised laboratories to ensure comparability across the network. To cope with the introduction of these new measurements, new reporting guidelines have been developed to ensure that all proper information about the methodologies and data quality is given.
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5.
  • Aas, Wenche, et al. (author)
  • Trends in Air Pollution in Europe, 2000–2019
  • 2024
  • In: Aerosol and Air Quality Research. - 2071-1409 .- 1680-8584. ; 24:4
  • Journal article (peer-reviewed)abstract
    • This paper encompasses an assessment of air pollution trends in rural environments in Europe over the 2000–2019 period, benefiting from extensive long-term observational data from the EMEP monitoring network and EMEP MSC-W model computations. The trends in pollutant concentrations align with the decreasing emission patterns observed throughout Europe. Annual average concentrations of sulfur dioxide, particulate sulfate, and sulfur wet deposition have shown consistent declines of 3–4% annually since 2000. Similarly, oxidized nitrogen species have markedly decreased across Europe, with an annual reduction of 1.5–2% in nitrogen dioxide concentrations, total nitrate in the air, and oxidized nitrogen deposition. Notably, emission reductions and model predictions appear to slightly surpass the observed declines in sulfur and oxidized nitrogen, indicating a potential overestimation of reported emission reductions. Ammonia emissions have decreased less compared to other pollutants since 2000. Significant reductions in particulate ammonium have however, been achieved due to the impact of reductions in SOx and NOx emissions. For ground level ozone, both the observed and modelled peak levels in summer show declining trends, although the observed decline is smaller than modelled. There have been substantial annual reductions of 1.8% and 2.4% in the concentrations of PM10 and PM2.5, respectively. Elemental carbon has seen a reduction of approximately 4.5% per year since 2000. A similar reduction for organic carbon is only seen in winter when primary anthropogenic sources dominate. The observed improvements in European air quality emphasize the importance of comprehensive legislations to mitigate emissions.
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6.
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7.
  • Angelbratt, Jon, 1981, et al. (author)
  • Carbon monoxide (CO) and ethane (C2H6) trends from ground-based solar FTIR measurements at six European stations, comparison and sensitivity analysis with the EMEP model
  • 2011
  • In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 11:17, s. 9253-9269
  • Journal article (peer-reviewed)abstract
    • Trends in the CO and C(2)H(6) partial columns (similar to 0-15 km) have been estimated from four European ground-based solar FTIR (Fourier Transform InfraRed) stations for the 1996-2006 time period. The CO trends from the four stations Jungfraujoch, Zugspitze, Harestua and Kiruna have been estimated to -0.45 +/- 0.16%yr(-1), -1.00 +/- 0.24%yr(-1), -0.62 +/- 0.19%yr(-1) and -0.61 +/- 0.16%yr(-1), respectively. The corresponding trends for C(2)H(6) are -1.51 +/- 0.23%yr(-1), -2.11 +/- 0.30%yr(-1), -1.09 +/- 0.25%yr(-1) and -1.14 +/- 0.18%yr(-1). All trends are presented with their 2-sigma confidence intervals. To find possible reasons for the CO trends, the global-scale EMEP MSC-W chemical transport model has been used in a series of sensitivity scenarios. It is shown that the trends are consistent with the combination of a 20% decrease in the anthropogenic CO emissions seen in Europe and North America during the 1996-2006 period and a 20% increase in the anthropogenic CO emissions in East Asia, during the same time period. The possible impacts of CH(4) and biogenic volatile organic compounds (BVOCs) are also considered. The European and global-scale EMEP models have been evaluated against the measured CO and C(2)H(6) partial columns from Jungfraujoch, Zugspitze, Bremen, Harestua, Kiruna and Ny-Alesund. The European model reproduces, on average the measurements at the different sites fairly well and within 10-22% deviation for CO and 14-31% deviation for C(2)H(6). Their seasonal amplitude is captured within 6-35% and 9-124% for CO and C(2)H(6), respectively. However, 61-98% of the CO and C(2)H(6) partial columns in the European model are shown to arise from the boundary conditions, making the global-scale model a more suitable alternative when modeling these two species. In the evaluation of the global model the average partial columns for 2006 are shown to be within 1-9% and 37-50% of the measurements for CO and C(2)H(6), respectively. The global model sensitivity for assumptions made in this paper is also analyzed.
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8.
  • Bergström, Robert, et al. (author)
  • Biotic stress: a significant contributor to organic aerosol in Europe?
  • 2014
  • In: Atmospheric Chemistry And Physics. - : Copernicus Publications. - 1680-7316 .- 1680-7324. ; 14:24, s. 13643-13660
  • Journal article (peer-reviewed)abstract
    • We have investigated the potential impact on organic aerosol formation from biotic stress-induced emissions (SIE) of organic molecules from forests in Europe (north of lat. 45° N). Emission estimates for sesquiterpenes (SQT), methyl salicylate (MeSA) and unsaturated C17 compounds, due to different stressors, are based on experiments in the Jülich Plant Atmosphere Chamber (JPAC), combined with estimates of the fraction of stressed trees in Europe based on reported observed tree damage. SIE were introduced in the EMEP MSC-W chemical transport model and secondary organic aerosol (SOA) yields from the SIE were taken from the JPAC experiments. Based on estimates of current levels of infestation and the JPAC aerosol yields, the model results suggest that the contribution to SOA in large parts of Europe may be substantial. It is possible that SIE contributes as much, or more, to organic aerosol than the constitutive biogenic VOC emissions, at least during some periods. Based on the assumptions in this study, SIE-SOA are estimated to constitute between 50 and 70 % of the total biogenic SOA (BSOA) in a current-situation scenario where the biotic stress in northern and central European forests causes large SIE of MeSA and SQT. An alternative current-situation scenario with lower SIE, consisting solely of SQT, leads to lower SIE-SOA, between 20 and 40 % of the total BSOA. Hypothetical future scenarios with increased SIE, due to higher degrees of biotic stress, show that SOA formation due to SIE can become even larger. Unsaturated C17 BVOC (biogenic volatile organic compounds) emitted by spruce infested by the forest-honey generating bark louse, Cinara pilicornis, have a high SOA-forming potential. A model scenario investigating the effect of a regional, episodic infestation of Cinara pilicornis in Baden-Württemberg, corresponding to a year with high production of forest honey, shows that these types of events could lead to very large organic aerosol formation in the infested region. We have used the best available laboratory data on biotic SIE applicable to northern and central European forests. Using these data and associated assumptions, we have shown that SIE are potentially important for SOA formation but the magnitude of the impact is uncertain and needs to be constrained by further laboratory, field and modelling studies. As an example, the MeSA, which is released as a consequence of various types of biotic stress, is found to have a potentially large impact on SIE-SOA in Europe, but different assumptions regarding the nighttime chemistry of MeSA can change its SOA potential substantially. Thus, further investigations of the atmospheric chemistry of MeSA and observational field studies are needed to clarify the role of this compound in the atmosphere.
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9.
  • Bergström, Robert, et al. (author)
  • Modelling of organic aerosols over Europe (2002-2007) using a volatility basis set (VBS) framework: application of different assumptions regarding the formation of secondary organic aerosol
  • 2012
  • In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 12:18, s. 8499-8527
  • Journal article (peer-reviewed)abstract
    • A new organic aerosol module has been implemented into the EMEP chemical transport model. Four different volatility basis set (VBS) schemes have been tested in long-term simulations for Europe, covering the six years 2002-2007. Different assumptions regarding partitioning of primary organic aerosol and aging of primary semi-volatile and intermediate volatility organic carbon (S/IVOC) species and secondary organic aerosol (SOA) have been explored. Model results are compared to filter measurements, aerosol mass spectrometry (AMS) data and source apportionment studies, as well as to other model studies. The present study indicates that many different sources contribute significantly to organic aerosol in Europe. Biogenic and anthropogenic SOA, residential wood combustion and vegetation fire emissions may all contribute more than 10% each over substantial parts of Europe. This study shows smaller contributions from biogenic SOA to organic aerosol in Europe than earlier work, but relatively greater anthropogenic SOA. Simple VBS based organic aerosol models can give reasonably good results for summer conditions but more observational studies are needed to constrain the VBS parameterisations and to help improve emission inventories. The volatility distribution of primary emissions is one important issue for further work. Emissions of volatile organic compounds from biogenic sources are also highly uncertain and need further validation. We can not reproduce winter levels of organic aerosol in Europe, and there are many indications that the present emission inventories substantially underestimate emissions from residential wood combustion in large parts of Europe.
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10.
  • Bessagnet, B., et al. (author)
  • Emissions of Carbonaceous Particulate Matter and Ultrafine Particles from Vehicles-A Scientific Review in a Cross-Cutting Context of Air Pollution and Climate Change
  • 2022
  • In: Applied Sciences (Switzerland). - : MDPI AG. - 2076-3417. ; 12:7
  • Research review (peer-reviewed)abstract
    • Featured Application Key conclusions and recommendations are proposed to enlighten decision makers in view of the next regulations on vehicle emissions in Europe and worldwide through the synergistic contexts of air quality and climate change. Airborne particulate matter (PM) is a pollutant of concern not only because of its adverse effects on human health but also on visibility and the radiative budget of the atmosphere. PM can be considered as a sum of solid/liquid species covering a wide range of particle sizes with diverse chemical composition. Organic aerosols may be emitted (primary organic aerosols, POA), or formed in the atmosphere following reaction of volatile organic compounds (secondary organic aerosols, SOA), but some of these compounds may partition between the gas and aerosol phases depending upon ambient conditions. This review focuses on carbonaceous PM and gaseous precursors emitted by road traffic, including ultrafine particles (UFP) and polycyclic aromatic hydrocarbons (PAHs) that are clearly linked to the evolution and formation of carbonaceous species. Clearly, the solid fraction of PM has been reduced during the last two decades, with the implementation of after-treatment systems abating approximately 99% of primary solid particle mass concentrations. However, the role of brown carbon and its radiative effect on climate and the generation of ultrafine particles by nucleation of organic vapour during the dilution of the exhaust remain unclear phenomena and will need further investigation. The increasing role of gasoline vehicles on carbonaceous particle emissions and formation is also highlighted, particularly through the chemical and thermodynamic evolution of organic gases and their propensity to produce particles. The remaining carbon-containing particles from brakes, tyres and road wear will still be a problem even in a future of full electrification of the vehicle fleet. Some key conclusions and recommendations are also proposed to support the decision makers in view of the next regulations on vehicle emissions worldwide.
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11.
  • Buker, P., et al. (author)
  • DO3SE modelling of soil moisture to determine ozone flux to forest trees
  • 2012
  • In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 12:12, s. 5537-5562
  • Journal article (peer-reviewed)abstract
    • The DO3SE (Deposition of O-3 for Stomatal Exchange) model is an established tool for estimating ozone (O-3) deposition, stomatal flux and impacts to a variety of vegetation types across Europe. It has been embedded within the EMEP (European Monitoring and Evaluation Programme) photochemical model to provide a policy tool capable of relating the flux-based risk of vegetation damage to O-3 precursor emission scenarios for use in policy formulation. A key limitation of regional flux-based risk assessments has been the assumption that soil water deficits are not limiting O-3 flux due to the unavailability of evaluated methods for modelling soil water deficits and their influence on stomatal conductance (g(sto)), and subsequent O-3 flux. This paper describes the development and evaluation of a method to estimate soil moisture status and its influence on g(sto) for a variety of forest tree species. This DO3SE soil moisture module uses the Penman-Monteith energy balance method to drive water cycling through the soil-plant-atmosphere system and empirical data describing g(sto) relationships with pre-dawn leaf water status to estimate the biological control of transpiration. We trial four different methods to estimate this biological control of the transpiration stream, which vary from simple methods that relate soil water content or potential directly to g(sto), to more complex methods that incorporate hydraulic resistance and plant capacitance that control water flow through the plant system. These methods are evaluated against field data describing a variety of soil water variables, g(sto) and transpiration data for Norway spruce (Picea abies), Scots pine (Pinus sylvestris), birch (Betula pendula), aspen (Populus tremuloides), beech (Fagus sylvatica) and holm oak (Quercus ilex) collected from ten sites across Europe and North America. Modelled estimates of these variables show consistency with observed data when applying the simple empirical methods, with the timing and magnitude of soil drying events being captured well across all sites and reductions in transpiration with the onset of drought being predicted with reasonable accuracy. The more complex methods, which incorporate hydraulic resistance and plant capacitance, perform less well, with predicted drying cycles consistently underestimating the rate and magnitude of water loss from the soil. A sensitivity analysis showed that model performance was strongly dependent upon the local parameterisation of key model drivers such as the maximum g(sto), soil texture, root depth and leaf area index. The results suggest that the simple modelling methods that relate g(sto) directly to soil water content and potential provide adequate estimates of soil moisture and influence on g(sto) such that they are suitable to be used to assess the potential risk posed by O-3 to forest trees across Europe.
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12.
  • Carrasco-Molina, Tania, et al. (author)
  • Validation and parametrization of the soil moisture index for stomatal conductance modelling and flux-based ozone risk assessment of Mediterranean plant species
  • 2024
  • In: Agricultural and Forest Meteorology. - 0168-1923. ; 354
  • Journal article (peer-reviewed)abstract
    • The Mediterranean region chronically experiences high levels of tropospheric ozone (O3) that can affect the health of vegetation. However, limiting plant growing conditions, such as low soil moisture, may restrict the stomatal phytotoxic ozone dose (POD) absorbed by vegetation, modulating O3 detrimental effects. Atmospheric chemistry transport models that estimate POD for O3 risk assessment of effects on vegetation species, such as the European Monitoring and Evaluation Programme (EMEP), have adopted the soil moisture index (SMI) to consider the influence of soil moisture on POD. The objectives of this study were the parametrization and validation of the SMI effect on stomatal conductance (gs) for improving the POD estimation and O3 risk assessment for different vegetation species under water-limiting growing conditions, using field data collected in Italy and Spain and a literature review. The modelled SMI from EMEP proved to be a good indicator of soil moisture dynamics across sites and years, although it showed a general tendency to overestimate soil moisture availability for plants, particularly in the driest seasons. New parametrizations derived for modelling SMI effects on gs under Mediterranean conditions proposed in this study stress the importance of using species-specific parameters for species showing contrasting water-saving strategies in contrast of the current approach of using a simple relation between SMI and gs for all the species. Furthermore, gs modelling parametrizations based on soil water potential (SWP) were found to be more suitable than SMI for local scale estimation of POD under water-limiting conditions. Further consideration of rooting depth and distribution will be required in the future to determine the soil depth at which the soil moisture should be measured in POD modelling, since these features represent one of the most important uncertainties affecting the estimation of POD that could not be addressed with the present database.
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13.
  • Clarke, N, et al. (author)
  • Availability, accessibility, quality and comparability of monitoring data for European forests for use in air pollution and climate change science
  • 2011
  • In: IForest. - : Italian Society of Sivilculture and Forest Ecology (SISEF). - 1971-7458. ; 4:1, s. 162-166
  • Journal article (peer-reviewed)abstract
    • Data from existing monitoring programmes such as ICP Forests, ICP Integrated Monitoring and EMEP, as well as from large-scale international projects such as CarboEurope IP and NitroEurope, can be used to answer questions about the impacts of air pollution and climate change on forest ecosystems and the feedbacks of forest to climate. However, for full use to be made of the available data, a number of questions need to be answered related to the availability, accessibility, quality and comparability of the data. For example, how can these databases be accessed, e.g., freely, over the internet, on request, by authorisation? How should intellectual property rights be protected, while improving access to data? What possibilities exist for harmonisation? Which quality assurance/quality control (QA/QC) procedures have been used and for how long? These and other relevant questions are discussed.
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14.
  • Colette, A., et al. (author)
  • Future air quality in Europe: a multi-model assessment of projected exposure to ozone
  • 2012
  • In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 12:21, s. 10613-10630
  • Journal article (peer-reviewed)abstract
    • In order to explore future air quality in Europe at the 2030 horizon, two emission scenarios developed in the framework of the Global Energy Assessment including varying assumptions on climate and energy access policies are investigated with an ensemble of six regional and global atmospheric chemistry transport models. A specific focus is given in the paper to the assessment of uncertainties and robustness of the projected changes in air quality. The present work relies on an ensemble of chemistry transport models giving insight into the model spread. Both regional and global scale models were involved, so that the ensemble benefits from medium-resolution approaches as well as global models that capture long-range transport. For each scenario a whole decade is modelled in order to gain statistical confidence in the results. A statistical downscaling approach is used to correct the distribution of the modelled projection. Last, the modelling experiment is related to a hind-cast study published earlier, where the performances of all participating models were extensively documented. The analysis is presented in an exposure-based framework in order to discuss policy relevant changes. According to the emission projections, ozone precursors such as NOx will drop down to 30% to 50% of their current levels, depending on the scenario. As a result, annual mean O-3 will slightly increase in NOx saturated areas but the overall O-3 burden will decrease substantially. Exposure to detrimental O-3 levels for health (SOMO35) will be reduced down to 45% to 70% of their current levels. And the fraction of stations where present-day exceedences of daily maximum O-3 is higher than 120 mu g m(-3) more than 25 days per year will drop from 43% down to 2 to 8 %. We conclude that air pollution mitigation measures (present in both scenarios) are the main factors leading to the improvement, but an additional cobenefit of at least 40% (depending on the indicator) is brought about by the climate policy.
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15.
  • de Vries, W., et al. (author)
  • Modelling long-term impacts of changes in climate, nitrogen deposition and ozone exposure on carbon sequestration of European forest ecosystems
  • 2017
  • In: Science of the Total Environment. - : Elsevier BV. - 0048-9697 .- 1879-1026. ; 605, s. 1097-1116
  • Journal article (peer-reviewed)abstract
    • We modelled the effects of past and expected future changes in climate (temperature, precipitation), CO2 concentration, nitrogen deposition (N) and ozone (O-3) exposure (phytotoxic ozone dose, POD) on carbon (C) sequestration by European forest ecosystems for the period 1900-2050. Tree C sequestration was assessed by using empirical response functions, while soil C sequestration was simulated with the process-based model VSD, combined with the RothC model. We evaluated two empirical growth responses to N deposition (linear and non-linear) and two O-3 exposure relationships (linear function with total biomass or net annual increment). We further investigated an 'interactive model' with interactions between drivers and a 'multiplicativemodel', in which the combined effect is the product of individual drivers. A single deposition and climate scenario was used for the period 1900-2050. Contrary to expectations, growth observations at European level for the period 1950-2010 compared better with predictions by the multiplicative model than with the interactive model. This coincides with the fact that carbon responses in kg C ha(-1) yr(-1) per unit change in drivers, i.e. per degrees C, ppm CO2, kg N ha(-1) yr(-1) and mmol m(-2) yr(-1) POD, aremore in line with literature data when using themultiplicativemodel. Compared to 1900, the estimated European average total C sequestration in both forests and forest soils between 1950 and 2000 increased by 21% in the interactive model and by 41% in the multiplicative model, but observed changes were even higher. This growth increase is expected to decline between 2000 and 2050. The simulated changes between 1950 and 2000 were mainly due to the increase in both N deposition and CO2, while the predicted increases between 2000 and 2050 were mainly caused by the increase in CO2 and temperature, and to lesser extent a decrease in POD, counteracted by reduced N deposition. (C) 2017 Elsevier B.V. All rights reserved.
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16.
  • de Vries, W., et al. (author)
  • Trends and geographic variation in adverse impacts of nitrogen use in Europe on human health, climate, and ecosystems: A review
  • 2024
  • In: Earth-Science Reviews. - 0012-8252. ; 253
  • Research review (peer-reviewed)abstract
    • This paper presents a review of the trends and geographic variation of impacts of reactive nitrogen (N) inputs on in Europe through impacts on air, soil and water quality. It illustrates those impacts, by assessing temporal and spatial variation in air, soil and water quality indicators and their exceedances of critical thresholds in view of impacts on human health, terrestrial and aquatic ecosystems, during 1990-2019. Trends are derived from regular inventory and monitoring data and from simulated trends in air quality using the EMEP model. Well quantified adverse impacts of increased N use are: (i) the effects on human health due to increased tropospheric concentrations of NOx and ozone, and N-induced increases in fine particulate matter, (ii) the contribution of N2O to climate change and stratospheric ozone depletion, (iii) the loss of plant and faunal diversity both in terrestrial and aquatic ecosystems via direct and soil mediated impacts, (iv) the acidification of forest soils, with impacts on tree forest nutrition, tree growth and tree vitality, and (v) the eutrophication of marine ecosystems, and associated biodiversity loss and occurrence of harmful algae blooms. Over the period 1990-2019, N inputs to agriculture stayed relatively constant, but the emissions of ammonia (NH3) decreased by 27%, while emissions of nitrogen oxides (NOx) decreased by 57%. In response to those reductions, concentrations of NOx, and of N in particulate matter also declined, although less than 50%. In contrast, the reduction in NOx-induced ozone concentrations and ozone related indicators (AOT40, SOMO35 and POD) was much less (ca 15-20%). Exceedances of critical ozone concentrations for human health and of critical AOT40 and POD vales for vegetation reduced in a similar order of magnitude. Despite decreasing NH3 emissions, NH3 concentrations showed a slight and steady increase from 1995 onwards, due to the large reduction in SOx emissions. Nitrogen deposition and exceedances of critical N loads for terrestrial ecosystems decreased by ca 60%, but the area exceeding critical N loads only reduced by ca 10%. Unlike N, the area exceeding critical acid loads has declined by more than 90% due to high reduction in SOx and NOx emissions. Trends in nitrate (NO3) concentrations in groundwater varied across Europe, but showed overall limited changes over the last two decades. However, N concentrations in surface water and the area exceeding critical levels in view of aquatic biodiversity has decreased and the same holds for N concentrations in coastal regions. Nevertheless, the eutrophication condition of coastal waters has overall not improved due to adverse impacts of elevated phosphorus inputs. Finally the negative impacts of N induced N2O emissions on climate are estimated to be outweighed by the positive effects of N induced CO2 sequestration, mainly in forests, and this holds for the whole period 1990-2019. Nitrogen hotspots, being areas with high exceedances in critical levels and loads of N compounds in air and water, are concentrated in intensive agricultural areas with high livestock densities and in urban region with strong industrial and traffic activities. Cost-benefit analysis shows that environmental costs of reactive N release to the environment are substantial and tend to exceed the direct economic benefits for agriculture. Given the relevance of N for safeguarding food production it is key to develop integrated and targeted plant nutrition strategies following a food system approach and practices that minimize trade-offs between productivity and the environment. In addition, targeted strategies to further reduce NOx emissions are needed to reduce air quality related health and biodiversity impacts.
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17.
  • Dore, A. J., et al. (author)
  • Evaluation and Inter-comparison of Acid Deposition Models for the UK
  • 2013
  • In: NATO Science for Peace and Security Series C: Environmental Security. - Dordrecht : Springer Netherlands. - 1874-6519. ; 137, s. 505-510
  • Journal article (peer-reviewed)abstract
    • An evaluation has been made of a range of simple and complex atmospheric transport models, applied to estimate sulphur and nitrogen deposition in the UK in order to provide information to policy makers to support decisions on future model use. The models were evaluated by comparison with annually averaged measurements from the national monitoring networks. A number of statistical metrics were output to assess model performance and the models were compared graphically by plotting cross-country transects of concentrations in air.
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18.
  • Dore, A. J., et al. (author)
  • Evaluation of the performance of different atmospheric chemical transport models and inter-comparison of nitrogen and sulphur deposition estimates for the UK
  • 2015
  • In: Atmospheric Environment. - : Elsevier BV. - 1873-2844 .- 1352-2310. ; 119, s. 131-143
  • Journal article (peer-reviewed)abstract
    • An evaluation has been made of a number of contrasting atmospheric chemical transport models, of varying complexity, applied to estimate sulphur and nitrogen deposition in the UK. The models were evaluated by comparison with annually averaged measurements of gas, aerosol and precipitation concentrations from the national monitoring networks. The models were evaluated in relation to performance criteria. They were generally able to satisfy a criterion of 'fitness for purpose' that at least 50% of modelled concentrations should be within a factor of two of measured values. The second criterion, that the magnitude of the normalised mean bias should be less than 20%, was not always satisfied. Considering known uncertainties in measurement techniques, this criterion may be too strict. Overall, simpler models were able to give a good representation of measured gas concentrations whilst the use of dynamic meteorology, and complex photo-chemical reactions resulted complex models. The models were compared graphically by plotting maps and cross-country transects of wet and dry deposition as well as calculating budgets of total wet and dry deposition to the UK for sulphur, oxidised nitrogen and reduced nitrogen. The total deposition to the UK varied by 22-36% amongst the different models depending on the deposition component. At a local scale estimates of both dry and wet deposition for individual 5 km x 5 km model grid squares were found to vary between the different models by up to a factor of 4.
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19.
  • Engardt, M., et al. (author)
  • Deposition of sulphur and nitrogen in Europe 1900-2050. Model calculations and comparison to historical observations
  • 2017
  • In: Tellus, Series B: Chemical and Physical Meteorology. - : Stockholm University Press. - 1600-0889 .- 0280-6509. ; 69:1, s. Article: 1328945-
  • Journal article (peer-reviewed)abstract
    • As a contribution to an EU project which dealt with the effects of climate change, air pollution impacts and ecosystems, two different atmospheric chemical transport models were used to simulate the depositions of acidifying and eutrophying pollutants over Europe for the period 1900-2050. Given the unavoidable uncertainties in the historical inputs to these simulations (emissions, meteorology), we generated a new and unique data-set for the purposes of model evaluation; comprising data from the European Air Chemistry Network (EACN) in operation from 1955 to early 1980s and more recent data from the EMEP monitoring network. The two models showed similar and reasonable skills in reproducing both the EACN and EMEP observational data although the MATCH model consistently simulates higher concentrations and depositions than the EMEP model. To further assess the models' ability to reproduce the long-term trend in sulphur and nitrogen deposition we compared modelled concentrations of major ions in precipitation with data extracted from a glacier in the European Alps. While, the shape and timing of the nss-sulphate data agrees reasonably, the ice core data indicate persistently high nitrogen concentrations of oxidised and reduced nitrogen after the 1980s which does not correspond to the model simulations or data from Western Europe in the EMEP monitoring network. This study concludes that nss-sulphate deposition to Europe was already clearly elevated in the year 1900, but has now (mid-2010s) decreased to about 70% of what it was at the beginning of the last century. The deposition of oxidised nitrogen to Europe peaked during the 1980s but has since decreased to half of its maximum value; still it is 3-4 times higher than in the year 1900. The annual deposition of reduced nitrogen to Europe is currently more than two times as high as the conditions in the year 1900.
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20.
  • Espen Yttri, Karl, et al. (author)
  • Trends, composition, and sources of carbonaceous aerosol at the Birkenes Observatory, northern Europe, 2001-2018
  • 2021
  • In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 21:9, s. 7149-7170
  • Journal article (peer-reviewed)abstract
    • We present 18 years (2001-2018) of aerosol measurements, including organic and elemental carbon (OC and EC), organic tracers (levoglucosan, arabitol, mannitol, trehalose, glucose, and 2-methyltetrols), trace elements, and ions, at the Birkenes Observatory (southern Norway) - a site representative of the northern European region. The OC=EC (2001-2018) and the levoglucosan (2008-2018) time series are the longest in Europe, with OC=EC available for the PM10, PM2:5 (fine), and PM10-2:5 (coarse) size fractions, providing the opportunity for a nearly 2-decade-long assessment. Using positive matrix factorization (PMF), we identify seven carbonaceous aerosol sources at Birkenes: mineraldust- dominated aerosol (MIN), traffic/industry-like aerosol (TRA/IND), short-range-transported biogenic secondary organic aerosol (BSOASRT), primary biological aerosol particles (PBAP), biomass burning aerosol (BB), ammoniumnitrate- dominated aerosol (NH4NO3), and (one low carbon fraction) sea salt aerosol (SS). We observed significant (p < 0:05), large decreases in EC in PM10 (-3:9%yr-1) and PM2:5 (-4:2%yr-1) and a smaller decline in levoglucosan (-2:8%yr-1), suggesting that OC=EC from traffic and industry is decreasing, whereas the abatement of OC=EC from biomass burning has been slightly less successful. EC abatement with respect to anthropogenic sources is further supported by decreasing EC fractions in PM2:5 (-3:9%yr-1) and PM10 (-4:5%yr-1). PMF apportioned 72% of EC to fossil fuel sources; this was further supported by PMF applied to absorption photometer data, which yielded a two-factor solution with a low aerosol ngstr m exponent (AAED0.93) fraction, assumed to be equivalent black carbon from fossil fuel combustion (eBCFF), contributing 78% to eBC mass. The higher AAE fraction (AAED2.04) is likely eBC from BB (eBCBB). Source-receptor model calculations (FLEXPART) showed that continental Europe and western Russia were the main source regions of both elevated eBCBB and eBCFF. Dominating biogenic sources explain why there was no downward trend for OC. A relative increase in the OC fraction in PM2:5 (C3:2%yr-1) and PM10 (C2:4%yr-1) underscores the importance of biogenic sources at Birkenes (BSOA and PBAP), which were higher in the vegetative season and dominated both fine (53 %) and coarse (78 %) OC. Furthermore, 77 %-91% of OC in PM2:5, PM10-2:5, and PM10 was attributed to biogenic sources in summer vs. 22 %- 37% in winter. The coarse fraction had the highest share of biogenic sources regardless of season and was dominated by PBAP, except in winter. Our results show a shift in the aerosol composition at Birkenes and, thus, also in the relative source contributions. The need for diverse offline and online carbonaceous aerosol speciation to understand carbonaceous aerosol sources, including their seasonal, annual, and long-term variability, has been demonstrated.
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21.
  • Etzold, Sophia, et al. (author)
  • Nitrogen deposition is the most important environmental driver of growth of pure, even-aged and managed European forests
  • 2020
  • In: Forest Ecology and Management. - : Elsevier BV. - 0378-1127 .- 1872-7042. ; 458
  • Journal article (peer-reviewed)abstract
    • Changing environmental conditions may substantially interact with site quality and forest stand characteristics, and impact forest growth and carbon sequestration. Understanding the impact of the various drivers of forest growth is therefore critical to predict how forest ecosystems can respond to climate change. We conducted a continental-scale analysis of recent (1995–2010) forest volume increment data (ΔVol, m3 ha−1 yr−1), obtained from ca. 100,000 coniferous and broadleaved trees in 442 even-aged, single-species stands across 23 European countries. We used multivariate statistical approaches, such as mixed effects models and structural equation modelling to investigate how European forest growth respond to changes in 11 predictors, including stand characteristics, climate conditions, air and site quality, as well as their interactions. We found that, despite the large environmental gradients encompassed by the forests examined, stand density and age were key drivers of forest growth. We further detected a positive, in some cases non-linear effect of N deposition, most pronounced for beech forests, with a tipping point at ca. 30 kg N ha−1 yr−1. With the exception of a consistent temperature signal on Norway spruce, climate-related predictors and ground-level ozone showed much less generalized relationships with ΔVol. Our results show that, together with the driving forces exerted by stand density and age, N deposition is at least as important as climate to modulate forest growth at continental scale in Europe, with a potential negative effect at sites with high N deposition.
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22.
  • Fischer, R, et al. (author)
  • Towards a transnational system of supersites for forest monitoring and research in Europe - an overview on present state and future recommendations
  • 2011
  • In: IForest. - : Italian Society of Sivilculture and Forest Ecology (SISEF). - 1971-7458. ; 4:1, s. 167-171
  • Journal article (peer-reviewed)abstract
    • Science based approaches in addressing future risks and challenges for forests require close collaboration among the communities operating different monitoring and research networks as well as experts in process and large-scale modelling. Results of the COST FP0903 conference which took place in October 2010 in Rome, reveal valuable results from different European forest monitoring and research networks. However, the need for closer integration of these activities is obvious. In this paper, representatives from major European networks recommend a new approach for forest monitoring and research in Europe, based on a reasonable number of highly instrumented "supersites" and a larger number of intensive monitoring plots linked to these. This system needs to be built on existing infrastructures but requires increased coordination, harmonisation and a joint long term platform for data exchange and modelling.
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23.
  • Flechard, C. R., et al. (author)
  • Advances in understanding, models and parameterizations of biosphere-atmosphere ammonia exchange
  • 2013
  • In: Biogeosciences. - : Copernicus GmbH. - 1726-4170 .- 1726-4189. ; 10:7, s. 5183-5225
  • Journal article (peer-reviewed)abstract
    • Atmospheric ammonia (NH3) dominates global emissions of total reactive nitrogen (N-r), while emissions from agricultural production systems contribute about two-thirds of global NH3 emissions; the remaining third emanates from oceans, natural vegetation, humans, wild animals and biomass burning. On land, NH3 emitted from the various sources eventually returns to the biosphere by dry deposition to sink areas, predominantly semi-natural vegetation, and by wet and dry deposition as ammonium (NH4+) to all surfaces. However, the land/atmosphere exchange of gaseous NH3 is in fact bi-directional over unfertilized as well as fertilized ecosystems, with periods and areas of emission and deposition alternating in time (diurnal, seasonal) and space (patchwork landscapes). The exchange is controlled by a range of environmental factors, including meteorology, surface layer turbulence, thermodynamics, air and surface heterogeneous-phase chemistry, canopy geometry, plant development stage, leaf age, organic matter decomposition, soil microbial turnover, and, in agricultural systems, by fertilizer application rate, fertilizer type, soil type, crop type, and agricultural management practices. We review the range of processes controlling NH3 emission and uptake in the different parts of the soil-canopy-atmosphere continuum, with NH3 emission potentials defined at the substrate and leaf levels by different [NH4+] / [H+] ratios (0).
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24.
  • Flechard, C. R., et al. (author)
  • Dry deposition of reactive nitrogen to European ecosystems: a comparison of inferential models across the NitroEurope network
  • 2011
  • In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 11:6, s. 2703-2728
  • Journal article (peer-reviewed)abstract
    • Inferential models have long been used to determine pollutant dry deposition to ecosystems from measurements of air concentrations and as part of national and regional atmospheric chemistry and transport models, and yet models still suffer very large uncertainties. An inferential network of 55 sites throughout Europe for atmospheric reactive nitrogen (N-r) was established in 2007, providing ambient concentrations of gaseous NH3, NO2, HNO3 and HONO and aerosol NH4+ and NO3- as part of the NitroEurope Integrated Project. Network results providing modelled inorganic Nr dry deposition to the 55 monitoring sites are presented, using four existing dry deposition routines, revealing inter-model differences and providing ensemble average deposition estimates. Dry deposition is generally largest over forests in regions with large ambient NH3 concentrations, exceeding 30-40 kg N ha(-1) yr(-1) over parts of the Netherlands and Belgium, while some remote forests in Scandinavia receive less than 2 kg N ha(-1) yr(-1). Turbulent Nr deposition to short vegetation ecosystems is generally smaller than to forests due to reduced turbulent exchange, but also because NH3 inputs to fertilised, agricultural systems are limited by the presence of a substantial NH3 source in the vegetation, leading to periods of emission as well as deposition. Differences between models reach a factor 2-3 and are often greater than differences between monitoring sites. For soluble Nr gases such as NH3 and HNO3, the non-stomatal pathways are responsible for most of the annual uptake over many surfaces, especially the non-agricultural land uses, but parameterisations of the sink strength vary considerably among models. For aerosol NH4+ and NO3-, discrepancies between theoretical models and field flux measurements lead to much uncertainty in dry deposition rates for fine particles (0.1-0.5 mu m). The validation of inferential models at the ecosystem scale is best achieved by comparison with direct long-term micrometeorological Nr flux measurements, but too few such datasets are available, especially for HNO3 and aerosol NH4+ and NO3-.
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25.
  • Fleming, Zoe L., et al. (author)
  • Tropospheric Ozone Assessment Report: Present-day ozone distribution and trends relevant to human health
  • 2018
  • In: Elementa. - : University of California Press. - 2325-1026. ; 6
  • Journal article (peer-reviewed)abstract
    • This study quantifies the present-day global and regional distributions (2010-2014) and trends (2000-2014) for five ozone metrics relevant for short-term and long-term human exposure. These metrics, calculated by the Tropospheric Ozone Assessment Report, are: 4th highest daily maximum 8-hour ozone (4MDA8); number of days with MDA8 > 70 ppb (NDGT70), SOMO35 (annual Sum of Ozone Means Over 35 ppb) and two seasonally averaged metrics (3MMDA1; AVGMDA8). These metrics were explored at ozone monitoring sites worldwide, which were classified as urban or non-urban based on population and nighttime lights data. Present-day distributions of 4MDA8 and NDGT70, determined predominantly by peak values, are similar with highest levels in western North America, southern Europe and East Asia. For the other three metrics, distributions are similar with North-South gradients more prominent across Europe and Japan. Between 2000 and 2014, significant negative trends in 4MDA8 and NDGT70 occur at most US and some European sites. In contrast, significant positive trends are found at many sites in South Korea and Hong Kong, with mixed trends across Japan. The other three metrics have similar, negative trends for many non-urban North American and some European and Japanese sites, and positive trends across much of East Asia. Globally, metrics at many sites exhibit non-significant trends. At 59% of all sites there is a common direction and significance in the trend across all five metrics, whilst 4MDA8 and NDGT70 have a common trend at similar to 80% of all sites. Sensitivity analysis shows AVGMDA8 trends differ with averaging period (warm season or annual). Trends are unchanged at many sites when a 1995-2014 period is used; although fewer sites exhibit non-significant trends. Over the longer period 1970-2014, most Japanese sites exhibit positive 4MDA8/SOMO35 trends. Insufficient data exist to characterize ozone trends for the rest of Asia and other world regions.
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26.
  • Fowler, D., et al. (author)
  • Atmospheric composition change : Ecosystems-Atmosphere interactions
  • 2009
  • In: Atmospheric Environment. - : Elsevier BV. - 1352-2310 .- 1873-2844. ; 43:33, s. 5193-5267
  • Research review (peer-reviewed)abstract
    • Ecosystems and the atmosphere: This review describes the state of understanding the processes involved in the exchange of trace gases and aerosols between the earth's surface and the atmosphere. The gases covered include NO, NO2, HONO, HNO3, NH3, SO2, DMS, Biogenic VOC, O-3, CH4, N2O and particles in the size range 1 nm-10 mu m including organic and inorganic chemical species. The main focus of the review is on the exchange between terrestrial ecosystems, both managed and natural and the atmosphere, although some new developments in ocean-atmosphere exchange are included. The material presented is biased towards the last decade, but includes earlier work, where more recent developments are limited or absent. New methodologies and instrumentation have enabled, if not driven technical advances in measurement. These developments have advanced the process understanding and upscaling of fluxes, especially for particles, VOC and NH3. Examples of these applications include mass spectrometric methods, such as Aerosol Mass Spectrometry (AMS) adapted for field measurement of atmosphere-surface fluxes using micrometeorological methods for chemically resolved aerosols. Also briefly described are some advances in theory and techniques in micrometeorology. For some of the compounds there have been paradigm shifts in approach and application of both techniques and assessment. These include flux measurements over marine surfaces and urban areas using micrometeorological methods and the up-scaling of flux measurements using aircraft and satellite remote sensing. The application of a flux-based approach in assessment of O-3 effects on vegetation at regional scales is an important policy linked development secured through improved quantification of fluxes. The coupling of monitoring, modelling and intensive flux measurement at a continental scale within the NitroEurope network represents a quantum development in the application of research teams to address the underpinning science of reactive nitrogen in the cycling between ecosystems and the atmosphere in Europe. Some important developments of the science have been applied to assist in addressing policy questions, which have been the main driver of the research agenda, while other developments in understanding have not been applied to their wider field especially in chemistry-transport models through deficiencies in obtaining appropriate data to enable application or inertia within the modelling community. The paper identifies applications, gaps and research questions that have remained intractable at least since 2000 within the specialized sections of the paper, and where possible these have been focussed on research questions for the coming decade. 
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27.
  • Fowler, D., et al. (author)
  • Effects of global change during the 21st century on the nitrogen cycle
  • 2015
  • In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 15:24, s. 13849-13893
  • Research review (peer-reviewed)abstract
    • The global nitrogen (N) cycle at the beginning of the 21st century has been shown to be strongly influenced by the inputs of reactive nitrogen (N-r) from human activities, including combustion-related NOx, industrial and agricultural N fixation, estimated to be 220 TgNyr(-1) in 2010, which is approximately equal to the sum of biological N fixation in unmanaged terrestrial and marine ecosystems. According to current projections, changes in climate and land use during the 21st century will increase both biological and anthropogenic fixation, bringing the total to approximately 600 TgNyr(-1) by around 2100. The fraction contributed directly by human activities is unlikely to increase substantially if increases in nitrogen use efficiency in agriculture are achieved and control measures on combustion-related emissions implemented. Some N-cycling processes emerge as particularly sensitive to climate change. One of the largest responses to climate in the processing of Nr is the emission to the atmosphere of NH3, which is estimated to increase from 65 TgNyr(-1) in 2008 to 93 TgNyr(-1) in 2100 assuming a change in global surface temperature of 5 degrees C in the absence of increased anthropogenic activity. With changes in emissions in response to increased demand for animal products the combined effect would be to increase NH3 emissions to 135 TgNyr(-1). Another major change is the effect of climate changes on aerosol composition and specifically the increased sublimation of NH4NO3 close to the ground to form HNO3 and NH3 in a warmer climate, which deposit more rapidly to terrestrial surfaces than aerosols. Inorganic aerosols over the polluted regions especially in Europe and North America were dominated by (NH4)(2)SO4 in the 1970s to 1980s, and large reductions in emissions of SO2 have removed most of the SO42- from the atmosphere in these regions. Inorganic aerosols from anthropogenic emissions are now dominated by NH4NO3, a volatile aerosol which contributes substantially to PM10 and human health effects globally as well as eutrophication and climate effects. The volatility of NH4NO3 and rapid dry deposition of the vapour phase dissociation products, HNO3 and NH3, is estimated to be reducing the transport distances, deposition footprints and inter-country exchange of N-r in these regions. There have been important policy initiatives on components of the global N cycle. These have been regional or country-based and have delivered substantial reductions of inputs of Nr to sensitive soils, waters and the atmosphere. To date there have been no attempts to develop a global strategy to regulate human inputs to the nitrogen cycle. However, considering the magnitude of global Nr use, potential future increases, and the very large leakage of Nr in many forms to soils, waters and the atmosphere, international action is required. Current legislation will not deliver the scale of reductions globally for recovery from the effects of Nr deposition on sensitive ecosystems, or a decline in N2O emissions to the global atmosphere. Such changes would require substantial improvements in nitrogen use efficiency across the global economy combined with optimization of transport and food consumption patterns. This would allow reductions in Nr use, inputs to the atmosphere and deposition to sensitive ecosystems. Such changes would offer substantial economic and environmental co-benefits which could help motivate the necessary actions.
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28.
  • Franz, Martina, et al. (author)
  • Development and evaluation of an ozone deposition scheme for coupling to a terrestrial biosphere model
  • 2017
  • In: Biogeosciences. - : Copernicus GmbH. - 1726-4170 .- 1726-4189. ; 14:1, s. 45-71
  • Journal article (peer-reviewed)abstract
    • Ozone (O3) is a toxic air pollutant that can damage plant leaves and substantially affect the plant's gross primary production (GPP) and health. Realistic estimates of the effects of tropospheric anthropogenic O3 on GPP are thus potentially important to assess the strength of the terrestrial biosphere as a carbon sink. To better understand the impact of ozone damage on the terrestrial carbon cycle, we developed a module to estimate O3 uptake and damage of plants for a state-of-the-art global terrestrial biosphere model called OCN. Our approach accounts for ozone damage by calculating (a) O3 transport from 45 m height to leaf level, (b) O3 flux into the leaf, and (c) ozone damage of photosynthesis as a function of the accumulated O3 uptake over the lifetime of a leaf. A comparison of modelled canopy conductance, GPP, and latent heat to FLUXNET data across European forest and grassland sites shows a general good performance of OCN including ozone damage. This comparison provides a good baseline on top of which ozone damage can be evaluated. In comparison to literature values, we demonstrate that the new model version produces realistic O3 surface resistances, O3 deposition velocities, and stomatal to total O3 flux ratios. A sensitivity study reveals that key metrics of the air-to-leaf O3 transport and O3 deposition, in particular the stomatal O3 uptake, are reasonably robust against uncertainty in the underlying parameterisation of the deposition scheme. Nevertheless, correctly estimating canopy conductance plays a pivotal role in the estimate of cumulative O3 uptake. We further find that accounting for stomatal and non-stomatal uptake processes substantially affects simulated plant O3 uptake and accumulation, because aerodynamic resistance and non-stomatal O3 destruction reduce the predicted leaf-level O3 concentrations. Ozone impacts on GPP and transpiration in a Europe-wide simulation indicate that tropospheric O3 impacts the regional carbon and water cycling less than expected from previous studies. This study presents a first step towards the integration of atmospheric chemistry and ecosystem dynamics modelling, which would allow for assessing the wider feedbacks between vegetation ozone uptake and tropospheric ozone burden.
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29.
  • Ge, Yao, et al. (author)
  • Evaluation of modelled versus observed non-methane volatile organic compounds at European Monitoring and Evaluation Programme sites in Europe
  • 2024
  • In: Atmospheric Chemistry and Physics. - 1680-7316 .- 1680-7324. ; 24:13, s. 7699-7729
  • Journal article (peer-reviewed)abstract
    • Atmospheric volatile organic compounds (VOCs) constitute a wide range of species, acting as precursors to ozone and aerosol formation. Atmospheric chemistry and transport models (CTMs) are crucial to understanding the emissions, distribution, and impacts of VOCs. Given the uncertainties in VOC emissions, lack of evaluation studies, and recent changes in emissions, this work adapts the European Monitoring and Evaluation Programme Meteorological Synthesizing Centre-West (EMEP MSC-W) CTM to evaluate emission inventories in Europe. Here we undertake the first intensive model-measurement comparison of VOCs in 2 decades. The modelled surface concentrations are evaluated both spatially and temporally, using measurements from the regular EMEP monitoring network in 2018 and 2019, as well as a 2022 campaign. To achieve this, we utilised the UK National Atmospheric Emissions Inventory to derive explicit emission profiles for individual species and employed a tracer method to produce pure concentrations that are directly comparable to observations. The degree to which the modelled and measured VOCs agree varies depending on the specific species. The model successfully captures the overall spatial and temporal variations of major alkanes (e.g. ethane, n-butane) and unsaturated species (e.g. ethene, benzene) but less so for propane, i-butane, and ethyne. This discrepancy underscores potential issues in the boundary conditions for the latter species and in their primary emissions from, in particular, the solvent and road transport sectors. Specifically, potential missing propane emissions and issues with its boundary conditions are highlighted by large model underestimations and smaller propane-To-ethane ratios compared to the measurement. Meanwhile, both the model and measurements show strong linear correlations among butane isomers and among pentane isomers, indicating common sources for these pairs of isomers. However, modelled ratios of i-butane to n-butane and i-pentane to n-pentane are approximately one-Third of the measured ratios, which is largely driven by significant emissions of n-butane and n-pentane from the solvent sector. This suggests issues with the speciation profile of the solvent sector, underrepresented contributions from transport and fuel evaporation sectors in current inventories, or both. Furthermore, the modelled ethene-To-ethyne and benzene-To-ethyne ratios differ significantly from measured ratios. The different model performance strongly points to shortcomings in the spatial and temporal patterns and magnitudes of ethyne emissions, especially during winter. For OVOCs, the modelled and measured concentrations of methanal and methylglyoxal show a good agreement, despite a moderate underestimation by the model in summer. This discrepancy could be attributed to an underestimation of contributions from biogenic sources or possibly a model overestimation of their photolytic loss in summer. However, the insufficiency of suitable measurements limits the evaluation of other OVOCs. Finally, model simulations employing the CAMS inventory show slightly better agreements with measurements than those using the Centre on Emission Inventories and Projections (CEIP) inventory. This enhancement is likely due to the CAMS inventory's detailed segmentation of the road transport sector, including its associated sub-sector-specific emission profiles. Given this improvement, alongside the previously mentioned concerns about the model's biased estimations of various VOC ratios, future efforts should focus on a more detailed breakdown of dominant emission sectors (e.g. solvents) and the refinement of their speciation profiles to improve model accuracy.
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30.
  • Gelencser, A., et al. (author)
  • Source apportionment of PM2.5 organic aerosol over Europe: Primary/secondary, natural/anthropogenic, and fossil/biogenic origin
  • 2007
  • In: Journal of Geophysical Research. - : American Geophysical Union (AGU). - 0148-0227 .- 2156-2202. ; 112:D23, s. 12-
  • Journal article (peer-reviewed)abstract
    • On the basis of a 2-year comprehensive data set obtained within the CARBOSOL project, seasonal source apportionment of PM2.5 aerosol is attempted for five rural/remote sites in Europe. The approach developed combines radiocarbon measurements with bulk measurements of organic carbon (OC), elemental carbon (EC), and two organic tracers ( levoglucosan and cellulose). Source types are lumped into primary emissions from fossil fuel combustion and biomass burning, bioaerosol, and secondary organic aerosol from precursors emitted by fossil and nonfossil sources. Bulk concentration ratios reported for these source types in the literature are used to estimate the source contributions which are constrained by measured radiocarbon concentrations. It has been found that while fossil-related sources predominate EC throughout the year at all sites, the sources of OC are primarily biogenic and markedly different between summer and winter. In winter biomass burning primary emission is the main source, with sizable additional contribution from fossil fuel combustion. In contrast, in summer secondary organic aerosol (SOA) from nonfossil sources becomes predominant (63-76% of TC), with some contribution of SOA from fossil fuel combustion. The results agree well with recent findings of other authors who established the predominance of biogenic SOA for rural sites in summer in Europe. An uncertainty analysis has been conducted, which shows that the main conclusions from this study are robust.
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31.
  • Genberg, Johan, et al. (author)
  • Light-absorbing carbon in Europe - measurement and modelling, with a focus on residential wood combustion emissions
  • 2013
  • In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 13:17, s. 8719-8738
  • Journal article (peer-reviewed)abstract
    • The atmospheric concentration of elemental carbon (EC) in Europe during the six-year period 2005-2010 has been simulated with the EMEP MSC-W model. The model bias compared to EC measurements was less than 20% for most of the examined sites. The model results suggest that fossil fuel combustion is the dominant source of EC in most of Europe but that there are important contributions also from residential wood burning during the cold seasons and, during certain episodes, also from open biomass burning (wildfires and agricultural fires). The modelled contributions from open biomass fires to ground level concentrations of EC were small at the sites included in the present study, <3% of the long-term average of EC in PM10. The modelling of this EC source is subject to many uncertainties, and it was likely underestimated for some episodes. EC measurements and modelled EC were also compared to optical measurements of black carbon (BC). The relationships between EC and BC (as given by mass absorption cross section, MAC, values) differed widely between the sites, and the correlation between observed EC and BC is sometimes poor, making it difficult to compare results using the two techniques and limiting the comparability of BC measurements to model EC results. A new bottom-up emission inventory for carbonaceous aerosol from residential wood combustion has been applied. For some countries the new inventory has substantially different EC emissions compared to earlier estimates. For northern Europe the most significant changes are much lower emissions in Norway and higher emissions in neighbouring Sweden and Finland. For Norway and Sweden, comparisons to source-apportionment data from winter campaigns indicate that the new inventory may improve model-calculated EC from wood burning. Finally, three different model setups were tested with variable atmospheric lifetimes of EC in order to evaluate the model sensitivity to the assumptions regarding hygroscopicity and atmospheric ageing of EC. The standard ageing scheme leads to a rapid transformation of the emitted hydrophobic EC to hygroscopic particles, and generates similar results when assuming that all EC is aged at the point of emission. Assuming hydrophobic emissions and no ageing leads to higher EC concentrations. For the more remote sites, the observed EC concentration was in between the modelled EC using standard ageing and the scenario treating EC as hydrophobic. This could indicate too-rapid EC ageing in the model in relatively clean parts of the atmosphere.
  •  
32.
  • Genberg, Johan, et al. (author)
  • Source apportionment of carbonaceous aerosol in southern Sweden
  • 2011
  • In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 11:22, s. 11387-11400
  • Journal article (peer-reviewed)abstract
    • A one-year study was performed at the Vavihill background station in southern Sweden to estimate the anthropogenic contribution to the carbonaceous aerosol. Weekly samples of the particulate matter PM10 were collected on quartz filters, and the amounts of organic carbon, elemental carbon, radiocarbon (14C) and levoglucosan were measured. This approach enabled source apportionment of the total carbon in the PM10 fraction using the concentration ratios of the sources. The sources considered in this study were emissions from the combustion of fossil fuels and biomass, as well as biogenic sources. During the summer, the carbonaceous aerosol mass was dominated by compounds of biogenic origin (80%), which are associated with biogenic primary and secondary organic aerosols. During the winter months, biomass combustion (32%) and fossil fuel combustion (28%) were the main contributors to the carbonaceous aerosol. Elemental carbon concentrations in winter were about twice as large as during summer, and can be attributed to biomass combustion, probably from domestic wood burning. The contribution of fossil fuels to elemental carbon was stable throughout the year, although the fossil contribution to organic carbon increased during the winter. Thus, the organic aerosol originated mainly from natural sources during the summer and from anthropogenic sources during the winter. The result of this source apportionment was compared with results from the EMEP MSC-W chemical transport model. The model and measurements were generally consistent for total atmospheric organic carbon, however, the contribution of the sources varied substantially. E.g. the biomass burning contributions of OC were underestimated by the model by a factor of 2.2 compared to the measurements.
  •  
33.
  • Glasius, M., et al. (author)
  • Composition and sources of carbonaceous aerosols in Northern Europe during winter
  • 2018
  • In: Atmospheric Environment. - : Elsevier BV. - 1873-2844 .- 1352-2310. ; 173, s. 127-141
  • Journal article (peer-reviewed)abstract
    • Sources of elemental carbon (EC) and organic carbon (OC) in atmospheric aerosols (carbonaceous aerosols) were investigated by collection of weekly aerosol filter samples at six background sites in Northern Europe (Birkenes, Norway; Vavihill, Sweden; Risoe, Denmark; Cabauw and Rotterdam in The Netherlands; Melpitz, Germany) during winter 2013. Analysis of 14 C and a set of molecular tracers were used to constrain the sources of EC and OC. During the four-week campaign, most sites (in particular those in Germany and The Netherlands) were affected by an episode during the first two weeks with high concentrations of aerosol, as continental air masses were transported westward. The analysis results showed a clear, increasing north to south gradient for most molecular tracers. Total carbon (TC = OC + EC) at Birkenes showed an average concentration of 0.5 ± 0.3 μg C m −3 , whereas the average concentration at Melpitz was 6.0 ± 4.3 μg C m −3 . One weekly mean TC concentration as high as 11 μg C m −3 was observed at Melpitz. Average levoglucosan concentrations varied by an order of magnitude from 25 ± 13 ng m −3 (Birkenes) to 249 ± 13 ng m −3 (Melpitz), while concentrations of tracers of fungal spores (arabitol and mannitol) and vegetative debris (cellulose) were very low, showing a minor influence of primary biological aerosol particles during the North European winter. The fraction of modern carbon generally varied from 0.57 (Melpitz) to 0.91 (Birkenes), showing an opposite trend compared to the molecular tracers and TC. Total concentrations of 10 biogenic and anthropogenic carboxylic acids, mainly of secondary origin, were 4–53 ng m −3 , with the lowest concentrations observed at Birkenes and the highest at Melpitz. However, the highest relative concentrations of carboxylic acids (normalized to TC) were observed at the most northern sites. Levels of organosulphates and nitrooxy organosulphates varied more than two orders of magnitude, from 2 to 414 ng m −3 , between individual sites and samples. The three sites Melpitz, Rotterdam and Cabauw, located closest to source regions in continental Europe, showed very high levels of organosulphates and nitrooxy organosulphates (up to 414 ng m −3 ) during the first two weeks of the study, while low levels ( < 7 ng m −3 ) were found at all sites except Melpitz during the last week. The large variation in organosulphate levels probably reflects differences in the presence of acidic sulphate aerosols, known from laboratory studies to accelerate the formation of these compounds. On average, the ratio of organic sulphate to inorganic sulphate was 1.5 ± 1.0% (range 0.1–3.4%). Latin-hypercube source apportionment techniques identified biomass burning as the major source of OC for all samples at all sites (typically > 40% of TC), while use and combustion of fossil fuels was the second most important source. Furthermore, EC from biomass burning accounted for 7–16% of TC, whereas EC from fossil sources contributed to < 2–23% of TC, of which the highest percentages were observed for low-concentration aerosol samples. Unresolved non-fossil sources (such as cooking and biogenic secondary organic aerosols) did not account for more than 5–12% of TC. The results confirm that wood combustion is a major source to OC and EC in Northern Europe during winter.
  •  
34.
  • Guarin, Jose Rafael, et al. (author)
  • Impacts of tropospheric ozone and climate change on Mexico wheat production
  • 2019
  • In: Climatic Change. - : Springer Science and Business Media LLC. - 1573-1480 .- 0165-0009. ; 155:2, s. 157-174
  • Journal article (peer-reviewed)abstract
    • Wheat is an important staple crop sensitive to negative effects from elevated tropospheric ozone (O 3 ) concentrations, but the impacts of future O 3 concentrations on wheat production in Mexico are unknown. To determine these impacts, the O 3 -modified DSSAT-NWheat crop model was used to simulate wheat production in Mexico using a baseline scenario with pre-industrial O 3 concentrations from 1980 to 2010 and five Global Climate Models (GCMs) under the Representative Concentration Pathway (RCP) 8.5 scenario from 2041 to 2070 paired with future O 3 concentrations from the European Monitoring and Evaluation Programme (EMEP) Meteorological Synthesizing Centre–West (MSC-W) model. Thirty-two representative major wheat-producing locations in Mexico were simulated assuming both irrigated and rainfed conditions for two O 3 sensitivity cultivar classifications. The simulations showed large variability (after averaging over 30 years) in yield loss, ranging from 7 to 26% because of O 3 impact, depending on the location, irrigation, and climate change emissions scenario. After upscaling and aggregating the simulations to the country scale based on observed irrigated and rainfed production, national wheat production for Mexico is expected to decline by 12% under the future RCP 8.5 climate change scenario with additional losses of 7 to 18% because of O 3 impact, depending on the cultivar O 3 sensitivity. This yield loss caused by O 3 is comparable with, or even larger than, the impact from projected future climatic change in temperature, rainfall, and atmospheric CO 2 concentration. Therefore, O 3 impacts should be considered in future agricultural impact assessments.
  •  
35.
  • Hallquist, Mattias, 1969, et al. (author)
  • Photochemical smog in China: scientific challenges and implications for air-quality policies
  • 2016
  • In: National Science Review. - : Oxford University Press (OUP). - 2095-5138 .- 2053-714X. ; 3:4, s. 401-403
  • Journal article (peer-reviewed)abstract
    • In large areas of China severe air pollution events pose a significant threat to human health, ecosystems and climate. Current reduction of primary emissions will also affect secondary pollutants such as ozone (O3) and particulate matter (PM), but the magnitude of the effects is uncertain. Major scientific challenges are related to the formation of O3 and secondary particulate matter including Secondary Organic Aerosols (SOA). Large uncertainties also remain regarding the interactions of soot, SOA and O3 under the influence of different SO2, NOX and VOC concentrations. To improve the understanding of these secondary atmospheric interactions in China, scientific areas of central importance for photochemically induced air pollutants have been identified. In addition to the scientific challenges, results from research need to be synthesized across several disciplines and communicated to stakeholders affected by air pollution and to policy makers responsible for developing abatement strategies. Development of these science-policy interactions can benefit from experience gained under the UN ECE Convention on Long Range Transboundary Air Pollution (LRTAP)
  •  
36.
  • Hallquist, Mattias, 1969, et al. (author)
  • The formation, properties and impact of secondary organic aerosol: Current and emerging issues
  • 2009
  • In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 9:14, s. 5155-5236
  • Journal article (peer-reviewed)abstract
    • Secondary organic aerosol (SOA) accounts for a significant fraction of ambient tropospheric aerosol and a detailed knowledge of the formation, properties and transformation of SOA is therefore required to evaluate its impact on atmospheric processes, climate and human health. The chemical and physical processes associated with SOA formation are complex and varied, and, despite considerable progress in recent years, a quantitative and predictive understanding of SOA formation does not exist and therefore represents a major research challenge in atmospheric science. This review begins with an update on the current state of knowledge on the global SOA budget and is followed by an overview of the atmospheric degradation mechanisms for SOA precursors, gas-particle partitioning theory and the analytical techniques used to determine the chemical composition of SOA. A survey of recent laboratory, field and modeling studies is also presented. The following topical and emerging issues are highlighted and discussed in detail: molecular characterization of biogenic SOA constituents, condensed phase reactions and oligomerization, the interaction of atmospheric organic components with sulfuric acid, the chemical and photochemical processing of organics in the atmospheric aqueous phase, aerosol formation from real plant emissions, interaction of atmospheric organic components with water, thermodynamics and mixtures in atmospheric models. Finally, the major challenges ahead in laboratory, field and modeling studies of SOA are discussed and recommendations for future research directions are proposed.
  •  
37.
  • Hertel, O., et al. (author)
  • Governing processes for reactive nitrogen compounds in the European atmosphere
  • 2012
  • In: Biogeosciences. - : Copernicus GmbH. - 1726-4170 .- 1726-4189. ; 9:12, s. 4921-4954
  • Research review (peer-reviewed)abstract
    • Reactive nitrogen (Nr) compounds have different fates in the atmosphere due to differences in the governing processes of physical transport, deposition and chemical transformation. N r compounds addressed here include reduced nitrogen (NH x : ammonia (NH 3 ) and its reaction product ammonium (NH 4 + )), oxidized nitrogen (NO y : nitrogen monoxide (NO) + nitrogen dioxide (NO 2 ) and their reaction products) as well as organic nitrogen compounds (organic N). Pollution abatement strategies need to take into account the differences in the governing processes of these compounds when assessing their impact on ecosystem services, biodiversity, human health and climate. NO x (NO + NO 2 ) emitted from traffic affects human health in urban areas where the presence of buildings increases the residence time in streets. In urban areas this leads to enhanced exposure of the population to NO x concentrations. NO x emissions generally have little impact on nearby ecosystems because of the small dry deposition rates of NO x . These compounds need to be converted into nitric acid (HNO 3 ) before removal through deposition is efficient. HNO 3 sticks quickly to any surface and is thereby either dry deposited or incorporated into aerosols as nitrate (NO 3 + ). In contrast to NOx compounds, NH 3 has potentially high impacts on ecosystems near the main agricultural sources of NH 3 because of its large ground-level concentrations along with large dry deposition rates. Aerosol phase NH 4 + and NO 3 + contribute significantly to background PM 2.5 and PM 10 (mass of aerosols with an aerodynamic diameter of less than 2.5 and 10 μm, respectively) with an impact on radiation balance as well as potentially on human health. Little is known quantitatively and qualitatively about organic N in the atmosphere, other than that it contributes a significant fraction of wet-deposited N, and is present in both gaseous and particulate forms. Further studies are needed to characterise the sources, air chemistry and removal rates of organic N emissions.
  •  
38.
  • Hodnebrog, O., et al. (author)
  • Impact of forest fires, biogenic emissions and high temperatures on the elevated Eastern Mediterranean ozone levels during the hot summer of 2007
  • 2012
  • In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 12:18, s. 8727-8750
  • Journal article (peer-reviewed)abstract
    • The hot summer of 2007 in southeast Europe has been studied using two regional atmospheric chemistry models; WRF-Chem and EMEP MSC-W. The region was struck by three heat waves and a number of forest fire episodes, greatly affecting air pollution levels. We have focused on ozone and its precursors using state-of-the-art inventories for anthropogenic, biogenic and forest fire emissions. The models have been evaluated against measurement data, and processes leading to ozone formation have been quantified. Heat wave episodes are projected to occur more frequently in a future climate, and therefore this study also makes a contribution to climate change impact research. The plume from the Greek forest fires in August 2007 is clearly seen in satellite observations of CO and NO2 columns, showing extreme levels of CO in and downwind of the fires. Model simulations reflect the location and influence of the fires relatively well, but the modelled magnitude of CO in the plume core is too low. Most likely, this is caused by underestimation of CO in the emission inventories, suggesting that the CO/NOx ratios of fire emissions should be re-assessed. Moreover, higher maximum values are seen in WRF-Chem than in EMEP MSC-W, presumably due to differences in plume rise altitudes as the first model emits a larger fraction of the fire emissions in the lowermost model layer. The model results are also in fairly good agreement with surface ozone measurements. Biogenic VOC emissions reacting with anthropogenic NOx emissions are calculated to contribute significantly to the levels of ozone in the region, but the magnitude and geographical distribution depend strongly on the model and biogenic emission module used. During the July and August heat waves, ozone levels increased substantially due to a combination of forest fire emissions and the effect of high temperatures. We found that the largest temperature impact on ozone was through the temperature dependence of the biogenic emissions, closely followed by the effect of reduced dry deposition caused by closing of the plants' stomata at very high temperatures. The impact of high temperatures on the ozone chemistry was much lower. The results suggest that forest fire emissions, and the temperature effect on biogenic emissions and dry deposition, will potentially lead to substantial ozone increases in a warmer climate.
  •  
39.
  • Jenkin, M. E., et al. (author)
  • The CRI v2.2 reduced degradation scheme for isoprene
  • 2019
  • In: Atmospheric Environment. - : Elsevier BV. - 1873-2844 .- 1352-2310. ; 212:1 Sept., s. 172-182
  • Journal article (peer-reviewed)abstract
    • The reduced representation of isoprene degradation in the Common Representative Intermediates (CRI)mechanism has been systematically updated, using the Master Chemical Mechanism (MCM v3.3.1)as a reference benchmark, with the updated mechanism being released as CRI v2.2. The complete isoprene degradation mechanism in CRI v2.2 consists of 186 reactions of 56 closed shell and free radical species, this being an order of magnitude reduction in size compared with MCM v3.3.1. The chemistry initiated by reaction with OH radicals, NO3 radicals and ozone (O3)is treated. An overview of the updates is provided, within the context of reported kinetic and mechanistic information. The revisions mainly relate to the OH-initiated chemistry, which tends to dominate under atmospheric conditions, although these include updates to the chemistry of products that are also generated from the O3- and NO3-initiated oxidation. The revisions have impacts in a number of key areas, including recycling of HOx and NOx. The performance of the CRI v2.2 isoprene mechanism has been compared with those of the preceding version (CRI v2.1)and the reference MCM v3.3.1 over a range of relevant conditions, using a box model of the tropical forested boundary layer. In addition, tests are carried out to ensure that the performance of MCM v3.3.1 remains robust to more recently reported information. CRI v2.2 has also been implemented into the STOCHEM chemistry-transport model, with a customized close-variant of CRI v2.2 implemented into the EMEP MSC-W chemistry-transport model. The results of these studies are presented and used to illustrate the global-scale impacts of the mechanistic updates on HOx radical concentrations.
  •  
40.
  • Jeričević, Amela, et al. (author)
  • The assessment of transboundary and regional air pollution due to particles
  • 2017
  • In: Airborne Particles: Origin, Emissions and Health Impacts. ; , s. 75-103
  • Book chapter (other academic/artistic)abstract
    • Elevated atmospheric particulate matter concentrations are associated with significant adverse health effects, affect ecosystems, influence visibility and cloud formation in the atmosphere and play an important role in climate change. Air quality modelling makes the connection between the design of effective mitigation strategies and knowledge of air pollutant sources. Transboundary and regional air quality models are one of the main scientific and policy tools used for the air quality assessment including particulate matter (PM). As sources outside cities often contribute significantly to local air pollution, many European cities will be unable to meet WHO guideline levels for air pollutants only by local action. Regional models resolve complex chemical processes of formation of secondary PM providing the possibility to identify the key mechanisms in their formation. Modelling results are primarily used to identify the contribution of the regional anthropogenic and natural emission sources of air pollution to the local levels, and to ensure high quality data for decision making that would jointly with the adequate measurements allow for the implementation of effective measures for air pollution reduction. The aim of this chapter is to provide an overview of transboundary and regional modelling of air pollution due to PM as well as the assessment of rural background PM measurements. Within this chapter regional model capabilities including input data (emissions, meteorology etc.) are discussed with focus on two widely applied atmospheric chemistry models EMEP and WRF/Chem as well as trajectory model Hysplit. Finally, the systematic review of some recent scientific papers focused on PM simulation and intercomparison of different models enabled the identification of unresolved scientific issues in regional PM simulations with atmospheric chemistry models.
  •  
41.
  • Jonson, J. E., et al. (author)
  • Impact of excess NOx emissions from diesel cars on air quality, public health and eutrophication in Europe
  • 2017
  • In: Environmental Research Letters. - : IOP Publishing. - 1748-9318 .- 1748-9326. ; 12:9
  • Journal article (peer-reviewed)abstract
    • Diesel cars have been emitting four to seven times more NOx in on-road driving than in type approval tests. These 'excess emissions' are a consequence of deliberate design of the vehicle's after-treatment system, as investigations during the 'Dieselgate' scandal have revealed. Here we calculate health and environmental impacts of these excess NOx emissions in all European countries for the year 2013. We use national emissions reported officially under the UNECE Convention for Long-range Transport of Atmospheric Pollutants and employ the EMEP MSC-W Chemistry Transport Model and the GAINS Integrated AssessmentModel to determine atmospheric concentrations and resulting impacts. We compare with impacts from hypothetical emissions where light duty diesel vehicles are assumed to emit only as much as their respective type approval limit value or as little as petrol cars of the same age. Excess NO2 concentrations can also have direct health impacts, but these overlap with the impacts from particulate matter ( PM) and are not included here. We estimate that almost 10 000 premature deaths from PM2.5 and ozone in the adult population (age>30 years) can be attributed to the NOx emissions from diesel cars and light commercial vehicles in EU28 plus Norway and Switzerland in 2013. About 50% of these could have been avoided if diesel limits had been achieved also in on-road driving; and had diesel cars emitted as little NOx as petrol cars, 80% of these premature deaths could have been avoided. Ecosystem eutrophication impacts (critical load exceedances) from the same diesel vehicles would also have been reduced at similar rates as for the health effects.
  •  
42.
  • Karl, M., et al. (author)
  • Uncertainties in assessing the environmental impact of amine emissions from a CO2 capture plant
  • 2014
  • In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 14:16, s. 8533-8557
  • Journal article (peer-reviewed)abstract
    • In this study, a new model framework that couples the atmospheric chemistry transport model system Weather Research and Forecasting-European Monitoring and Evaluation Programme (WRF-EMEP) and the multimedia fugacity level III model was used to assess the environmental impact of in-air amine emissions from post-combustion carbon dioxide capture. The modelling framework was applied to a typical carbon capture plant artificially placed at Mongstad, on the west coast of Norway. The study region is characterized by high precipitation amounts, relatively few sunshine hours, predominantly westerly winds from the North Atlantic and complex topography. Mongstad can be considered as moderately polluted due to refinery activities. WRF-EMEP enables a detailed treatment of amine chemistry in addition to atmospheric transport and deposition. Deposition fluxes of WRF-EMEP simulations were used as input to the fugacity model in order to derive concentrations of nitramines and nitrosamine in lake water. Predicted concentrations of nitramines and nitrosamines in ground-level air and drinking water were found to be highly sensitive to the description of amine chemistry, especially of the night-time chemistry with the nitrate (NO3) radical. Sensitivity analysis of the fugacity model indicates that catchment characteristics and chemical degradation rates in soil and water are among the important factors controlling the fate of these compounds in lake water. The study shows that realistic emission of commonly used amines result in levels of the sum of nitrosamines and nitramines in ground-level air (0.6-10 pgm(-3)) and drinking water (0.04-0.25 ng L-1) below the current safety guideline for human health that is enforced by the Norwegian Environment Agency. The modelling framework developed in this study can be used to evaluate possible environmental impacts of emissions of amines from post-combustion capture in other regions of the world.
  •  
43.
  • Karlsson, Per Erik, 1957, et al. (author)
  • Ozone Exposure and Impacts on Vegetation in the Nordic and Baltic Countries
  • 2009
  • In: Ambio. - : Royal Swedish Academy of Sciences. - 0044-7447 .- 1654-7209. ; 38:8, s. 402-405
  • Journal article (peer-reviewed)abstract
    • Ozone concentrations are generally considerably lower over northern Europe as compared with continental and southern Europe. However, ozone becomes toxic for vegetation mainly after it has been taken up into the leaf interior through the stomata. The rates of ozone uptake into the leaves are, somewhat simplified, the product of the air ozone concentrations and the degree of stomatal opening. The phytotoxic impacts of ozone can be almost as important in northern Europe as they are in continental and southern Europe. The long daylight hours as well as the rather humid environment conditions, both in the air and soil, promote stomatal openings in northern Europe. This article summarizes scientific evidence that supports the conclusion that ozone abatement policies regarding vegetation in Europe, as well as in the rest of the world, should be based on estimates of the leaf ozone uptake and not only on the ozone concentration in the air.
  •  
44.
  • Klingberg, Jenny, 1978, et al. (author)
  • Comparison of modelled and measured ozone concentrations and meteorology for a site in south-west Sweden: Implications for ozone uptake calculations
  • 2008
  • In: Environmental Pollution. - : Elsevier BV. - 0269-7491 .- 1873-6424. ; 155:1, s. 99-111
  • Journal article (peer-reviewed)abstract
    • Measurements of ground-level ozone concentrations and meteorology (temperature, vapour pressure deficit (VPD), solar radiation) at the monitoring site Ostad (south-west Sweden) were compared to data from the corresponding grid in the EMEP photo-oxidant model for 1997, 1999 and 2000. The influence of synoptic weather on the agreement between model and measurements was studied. Implications of differences between modelled and observed inputs for ozone flux calculations for wheat and potato were investigated. The EMEP model output of ozone, temperature and VPD correlated well with measurements during daytime. Deviations were larger during the night, especially in calm conditions, attributed to local climatological conditions at the monitoring site deviating from average conditions of the grid. These differences did not lead to significant differences in calculated ozone uptake, which was reproduced remarkably well. The uptake calculations were sensitive to errors in the ozone and temperature input data, especially when including a flux threshold. (C) 2007 Elsevier Ltd. All rights reserved.
  •  
45.
  • Kulmala, M., et al. (author)
  • General overview: European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) - integrating aerosol research from nano to global scales
  • 2011
  • In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 11:24, s. 13061-13143
  • Journal article (peer-reviewed)abstract
    • In this paper we describe and summarize the main achievements of the European Aerosol Cloud Climate and Air Quality Interactions project (EUCAARI). EUCAARI started on 1 January 2007 and ended on 31 December 2010 leaving a rich legacy including: (a) a comprehensive database with a year of observations of the physical, chemical and optical properties of aerosol particles over Europe, (b) comprehensive aerosol measurements in four developing countries, (c) a database of airborne measurements of aerosols and clouds over Europe during May 2008, (d) comprehensive modeling tools to study aerosol processes fron nano to global scale and their effects on climate and air quality. In addition a new Pan-European aerosol emissions inventory was developed and evaluated, a new cluster spectrometer was built and tested in the field and several new aerosol parameterizations and computations modules for chemical transport and global climate models were developed and evaluated. These achievements and related studies have substantially improved our understanding and reduced the uncertainties of aerosol radiative forcing and air quality-climate interactions. The EUCAARI results can be utilized in European and global environmental policy to assess the aerosol impacts and the corresponding abatement strategies.
  •  
46.
  • Laj, P., et al. (author)
  • Measuring Atmospheric Composition Change
  • 2009
  • In: Atmospheric Environment. - : Elsevier BV. - 1873-2844 .- 1352-2310. ; 43:33, s. 5351-5414
  • Journal article (peer-reviewed)abstract
    • Scientific findings from the last decades have clearly highlighted the need for a more comprehensive approach to atmospheric change processes. In fact, observation of atmospheric composition variables has been an important activity of atmospheric research that has developed instrumental tools (advanced analytical techniques) and platforms (instrumented passenger aircrafts, ground-based in-situ and remote sensing stations, earth observation satellite instruments) providing essential information on the composition of the atmosphere. The variability of the atmospheric system and the extreme complexity of the atmospheric cycles for short-lived gaseous and aerosol species have led to the development of complex models to interpret observations, test our theoretical understanding of atmospheric chemistry and predict future atmospheric composition. The validation of numerical models requires accurate information concerning the variability of atmospheric composition for targeted species via comparison with observations and measurements. In this paper, we provide an overview of recent advances in instrumentation and methodologies for measuring atmospheric composition changes from space, aircraft and the surface as well as recent improvements in laboratory techniques that permitted scientific advance in the field of atmospheric chemistry. Emphasis is given to the most promising and innovative technologies that will become operational in the near future to improve knowledge of atmospheric composition. Our current observation capacity, however, is not satisfactory to understand and predict future atmospheric composition changes, in relation to predicted climate warming. Based on the limitation of the current European observing system, we address the major gaps in a second part of the paper to explain why further developments in current observation strategies are still needed to strengthen and optimise an observing system not only capable of responding to the requirements of atmospheric services but also to newly open scientific questions.
  •  
47.
  • Langner, J., et al. (author)
  • A multi-model study of impacts of climate change on surface ozone in Europe
  • 2012
  • In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 12:21, s. 10423-10440
  • Journal article (peer-reviewed)abstract
    • 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 20002009 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 O-3 could be especially important in connection with extreme summer events.
  •  
48.
  • Le Breton, Michael, 1986, et al. (author)
  • Chlorine oxidation of VOCs at a semi-rural site in Beijing: significant chlorine liberation from ClNO2 and subsequent gas- and particle-phase Cl-VOC production
  • 2018
  • In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 18:17, s. 13013-13030:18, s. 13013-13030
  • Journal article (peer-reviewed)abstract
    • Nitryl chloride (ClNO2) accumulation at night acts as a significant reservoir for active chlorine and impacts the following day's photochemistry when the chlorine atom is liberated at sunrise. Here, we report simultaneous measurements of N2O5 and a suite of inorganic halogens including ClNO2 and reactions of chloride with volatile organic compounds (Cl-VOCs) in the gas and particle phases utilising the Filter Inlet for Gas and AEROsols time-of-flight chemical ionisation mass spectrometer (FIGAERO-ToF-CIMS) during an intensive measurement campaign 40 km northwest of Beijing in May and June 2016. A maximum mixing ratio of 2900 ppt of ClNO2 was observed with a mean campaign nighttime mixing ratio of 487 ppt, appearing to have an anthropogenic source supported by correlation with SO2, CO and benzene, which often persisted at high levels after sunrise until midday. This was attributed to such high mixing ratios persisting after numerous e-folding times of the photolytic lifetime enabling the chlorine atom production to reach 2.3 x 10(5) molecules cm(-3) from ClNO2 alone, peaking at 09:30 LT and up to 8.4 x 10(5) molecules cm(-3) when including the supporting inorganic halogen measurements. Cl-VOCs were observed in the particle and gas phases for the first time at high time resolution and illustrate how the iodide ToF-CIMS can detect unique markers of chlorine atom chemistry in ambient air from both biogenic and anthropogenic sources. Their presence and abundance can be explained via time series of their measured and steady-state calculated precursors, enabling the assessment of competing OH and chlorine atom oxidation via measurements of products from both of these mechanisms and their relative contribution to secondary organic aerosol (SOA) formation.
  •  
49.
  • Leip, A., et al. (author)
  • Impacts of European livestock production: nitrogen, sulphur, phosphorus and greenhouse gas emissions, land-use, water eutrophication and biodiversity
  • 2015
  • In: Environmental Research Letters. - : IOP Publishing. - 1748-9318 .- 1748-9326. ; 10:11
  • Journal article (peer-reviewed)abstract
    • Livestock production systems currently occupy around 28% of the land surface of the European Union (equivalent to 65% of the agricultural land). In conjunction with other human activities, livestock production systems affect water, air and soil quality, global climate and biodiversity, altering the biogeochemical cycles of nitrogen, phosphorus and carbon. Here, we quantify the contribution of European livestock production to these major impacts. For each environmental effect, the contribution of livestock is expressed as shares of the emitted compounds and land used, as compared to the whole agricultural sector. The results show that the livestock sector contributes significantly to agricultural environmental impacts. This contribution is 78% for terrestrial biodiversity loss, 80% for soil acidification and air pollution (ammonia and nitrogen oxides emissions), 81% for global warming, and 73% for water pollution (both N and P). The agriculture sector itself is one of the major contributors to these environmental impacts, ranging between 12% for global warming and 59% for N water quality impact. Significant progress in mitigating these environmental impacts in Europe will only be possible through a combination of technological measures reducing livestock emissions, improved food choices and reduced food waste of European citizens.
  •  
50.
  • Lukacs, H., et al. (author)
  • Seasonal trends and possible sources of brown carbon based on 2-year aerosol measurements at six sites in Europe
  • 2007
  • In: Journal of Geophysical Research. - : American Geophysical Union (AGU). - 0148-0227 .- 2156-2202. ; 112:D23, s. 9-
  • Journal article (peer-reviewed)abstract
    • Brown carbon is a ubiquitous and unidentified component of organic aerosol which has recently come into the forefront of atmospheric research. This component is strongly linked to the class of humic-like substances (HULIS) in aerosol whose ultimate origin is still being debated. Using a simplified spectroscopic method the concentrations of brown carbon have been determined in aqueous extracts of fine aerosol collected during the CARBOSOL project. On the basis of the results of 2-year measurements of several aerosol constituents at six European sites, possible sources of brown carbon are inferred. Biomass burning ( possibly domestic wood burning) is shown to be a major source of brown carbon in winter. At elevated sites in spring, smoke from agricultural fires may be an additional source. Direct comparison of measured brown carbon concentrations with HULIS determined by an independent method reveals that the two quantities correlate well at low-elevation sites throughout the year. At high-elevation sites the correlation is still high for winter but becomes markedly lower in summer, implying different sources and/or atmospheric sinks of brown carbon and HULIS. The results shed some light on the relationships between atmospheric brown carbon and HULIS, two ill-defined and overlapping components of organic aerosol.
  •  
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Simpson, David, 1961 (92)
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