Improving Estimates of Sulfur, Nitrogen, and Ozone Total Deposition through Multi-Model and Measurement-Model Fusion Approaches.

Earth system and environmental impact studies need high quality and up-to-date estimates of atmospheric deposition. This study demonstrates the methodological benefits of multimodel ensemble and measurement-model fusion mapping approaches for atmospheric deposition focusing on 2010, a year for which several studies were conducted. Global model-only deposition assessment can be further improved by integrating new model-measurement techniques, including expanded capabilities of satellite observations of atmospheric composition. We identify research and implementation priorities for timely estimates of deposition globally as implemented by the World Meteorological Organization.

Lower air pollution during COVID-19 lock-down: improving models and methods estimating ozone impacts on crops.

We suggest that the unprecedented and unintended decrease of emissions of air pollutants during the COVID-19 lock-down in 2020 could lead to declining seasonal ozone concentrations and positive impacts on crop yields. An initial assessment of the potential effects of COVID-19 emission reductions was made using a set of six scenarios that variously assumed annual European and global emission reductions of 30% and 50% for the energy, industry, road transport and international shipping sectors, and 80% for the aviation sector. The greatest ozone reductions during the growing season reached up to 12 ppb over crop growing regions in Asia and up to 6 ppb in North America and Europe for the 50% global reduction scenario. In Europe, ozone responses are more sensitive to emission declines in other continents, international shipping and aviation than to emissions changes within Europe. We demonstrate that for wheat the overall magnitude of ozone precursor emission changes could lead to yield improvements between 2% and 8%. The expected magnitude of ozone precursor emission reductions during the Northern Hemisphere growing season in 2020 presents an opportunity to test and improve crop models and experimentally based exposure response relationships of ozone impacts on crops, under real-world conditions. This article is part of a discussion meeting issue 'Air quality, past present and future'.

Ozone pollution will compromise efforts to increase global wheat production.

Introduction of high-performing crop cultivars and crop/soil water management practices that increase the stomatal uptake of carbon dioxide and photosynthesis will be instrumental in realizing the United Nations Sustainable Development Goal (SDG) of achieving food security. To date, however, global assessments of how to increase crop yield have failed to consider the negative effects of tropospheric ozone, a gaseous pollutant that enters the leaf stomatal pores of plants along with carbon dioxide, and is increasing in concentration globally, particularly in rapidly developing countries. Earlier studies have simply estimated that the largest effects are in the areas with the highest ozone concentrations. Using a modelling method that accounts for the effects of soil moisture deficit and meteorological factors on the stomatal uptake of ozone, we show for the first time that ozone impacts on wheat yield are particularly large in humid rain-fed and irrigated areas of major wheat-producing countries (e.g. United States, France, India, China and Russia). Averaged over 2010-2012, we estimate that ozone reduces wheat yields by a mean 9.9% in the northern hemisphere and 6.2% in the southern hemisphere, corresponding to some 85 Tg (million tonnes) of lost grain. Total production losses in developing countries receiving Official Development Assistance are 50% higher than those in developed countries, potentially reducing the possibility of achieving UN SDG2. Crucially, our analysis shows that ozone could reduce the potential yield benefits of increasing irrigation usage in response to climate change because added irrigation increases the uptake and subsequent negative effects of the pollutant. We show that mitigation of air pollution in a changing climate could play a vital role in achieving the above-mentioned UN SDG, while also contributing to other SDGs related to human health and well-being, ecosystems and climate change.

"What We Breathe Impacts Our Health: Improving Understanding of the Link between Air Pollution and Health".

Air pollution contributes to the premature deaths of millions of people each year around the world, and air quality problems are growing in many developing nations. While past policy efforts have succeeded in reducing particulate matter and trace gases in North America and Europe, adverse health effects are found at even these lower levels of air pollution. Future policy actions will benefit from improved understanding of the interactions and health effects of different chemical species and source categories. Achieving this new understanding requires air pollution scientists and engineers to work increasingly closely with health scientists. In particular, research is needed to better understand the chemical and physical properties of complex air pollutant mixtures, and to use new observations provided by satellites, advanced in situ measurement techniques, and distributed micro monitoring networks, coupled with models, to better characterize air pollution exposure for epidemiological and toxicological research, and to better quantify the effects of specific source sectors and mitigation strategies.

Ambient Air Pollution Exposure Estimation for the Global Burden of Disease 2013.

Exposure to ambient air pollution is a major risk factor for global disease. Assessment of the impacts of air pollution on population health and evaluation of trends relative to other major risk factors requires regularly updated, accurate, spatially resolved exposure estimates. We combined satellite-based estimates, chemical transport model simulations, and ground measurements from 79 different countries to produce global estimates of annual average fine particle (PM2.5) and ozone concentrations at 0.1° × 0.1° spatial resolution for five-year intervals from 1990 to 2010 and the year 2013. These estimates were applied to assess population-weighted mean concentrations for 1990-2013 for each of 188 countries. In 2013, 87% of the world's population lived in areas exceeding the World Health Organization Air Quality Guideline of 10 µg/m(3) PM2.5 (annual average). Between 1990 and 2013, global population-weighted PM2.5 increased by 20.4% driven by trends in South Asia, Southeast Asia, and China. Decreases in population-weighted mean concentrations of PM2.5 were evident in most high income countries. Population-weighted mean concentrations of ozone increased globally by 8.9% from 1990-2013 with increases in most countries-except for modest decreases in North America, parts of Europe, and several countries in Southeast Asia.

Exposure assessment for estimation of the global burden of disease attributable to outdoor air pollution.

Ambient air pollution is associated with numerous adverse health impacts. Previous assessments of global attributable disease burden have been limited to urban areas or by coarse spatial resolution of concentration estimates. Recent developments in remote sensing, global chemical-transport models, and improvements in coverage of surface measurements facilitate virtually complete spatially resolved global air pollutant concentration estimates. We combined these data to generate global estimates of long-term average ambient concentrations of fine particles (PM(2.5)) and ozone at 0.1° × 0.1° spatial resolution for 1990 and 2005. In 2005, 89% of the world's population lived in areas where the World Health Organization Air Quality Guideline of 10 µg/m(3) PM(2.5) (annual average) was exceeded. Globally, 32% of the population lived in areas exceeding the WHO Level 1 Interim Target of 35 µg/m(3), driven by high proportions in East (76%) and South (26%) Asia. The highest seasonal ozone levels were found in North and Latin America, Europe, South and East Asia, and parts of Africa. Between 1990 and 2005 a 6% increase in global population-weighted PM(2.5) and a 1% decrease in global population-weighted ozone concentrations was apparent, highlighted by increased concentrations in East, South, and Southeast Asia and decreases in North America and Europe. Combined with spatially resolved population distributions, these estimates expand the evaluation of the global health burden associated with outdoor air pollution.

Atmospheric transport and deposition of mineral dust to the ocean: implications for research needs.

This paper reviews our knowledge of the measurement and modeling of mineral dust emissions to the atmosphere, its transport and deposition to the ocean, the release of iron from the dust into seawater, and the possible impact of that nutrient on marine biogeochemistry and climate. Of particular concern is our poor understanding of the mechanisms and quantities of dust deposition as well as the extent of iron solubilization from the dust once it enters the ocean. Model estimates of dust deposition in remote oceanic regions vary by more than a factor of 10. The fraction of the iron in dust that is available for use by marine phytoplankton is still highly uncertain. There is an urgent need for a long-term marine atmospheric surface measurement network, spread across all oceans. Because the southern ocean is characterized by large areas with high nitrate but low chlorophyll surface concentrations, that region is particularly sensitive to the input of dust and iron. Data from this region would be valuable, particularly at sites downwind from known dust source areas in South America, Australia, and South Africa. Coordinated field experiments involving both atmospheric and marine measurements are recommended to address the complex and interlinked processes and role of dust/Fe fertilization on marine biogeochemistry and climate.

Estimating resilience of crop production systems: From theory to practice.

Agricultural production systems are sensitive to weather and climate anomalies and extremes as well as to other environmental and socio-economic adverse events. An adequate evaluation of the resilience of such systems helps to assess food security and the capacity of society to cope with the effects of global warming and the associated increase of climate extremes. Here, we propose and apply a simple indicator of resilience of annual crop production that can be estimated from crop production time series. First, we address the problem of quantifying resilience in a simplified theoretical framework, focusing on annual crops. This results in the proposal of an indicator, measured by the reciprocal of the squared coefficient of variance, which is proportional to the return period of the largest shocks that the crop production system can absorb, and which is consistent with the original ecological definition of resilience. Subsequently, we show the sensitivity of the crop resilience indicator to the level of management of the crop production system, to the frequency of extreme events as well as to simplified socio-economic impacts of the production losses. Finally, we demonstrate the practical applicability of the indicator using historical production data at national and sub-national levels for France. The results show that the value of the resilience indicator steeply increases with crop diversity until six crops are considered, and then levels off. The effect of diversity on production resilience is highest when crops are more diverse (i.e. as reflected in less well correlated production time series). In the case of France, the indicator reaches about 60% of the value that would be expected if all crop production time-series were uncorrelated.

Narrowing uncertainties in the effects of elevated CO2 on crops.

Plant responses to rising atmospheric carbon dioxide (CO2) concentrations, together with projected variations in temperature and precipitation will determine future agricultural production. Estimates of the impacts of climate change on agriculture provide essential information to design effective adaptation strategies, and develop sustainable food systems. Here, we review the current experimental evidence and crop models on the effects of elevated CO2 concentrations. Recent concerted efforts have narrowed the uncertainties in CO2-induced crop responses so that climate change impact simulations omitting CO2 can now be eliminated. To address remaining knowledge gaps and uncertainties in estimating the effects of elevated CO2 and climate change on crops, future research should expand experiments on more crop species under a wider range of growing conditions, improve the representation of responses to climate extremes in crop models, and simulate additional crop physiological processes related to nutritional quality.

Soil sensitivity to acidification in Asia: status and prospects.

Exceedance of steady-state critical loads for soil acidification is consistently found in southern China and parts of SE Asia, but there is no evidence of impacts outside of China. This study describes a methodology for calculating the time to effects for soils sensitive to acidic deposition in Asia under potential future sulfur (S), nitrogen (N), and calcium (Ca) emission scenarios. The calculations are matched to data availability in Asia to produce regional-scale maps that provide estimates of the time (y) it will take for soil base saturation to reach a critical limit of 20% in response to acidic inputs. The results show that sensitive soil types in areas of South, Southeast, and East Asia, including parts of southern China, Burma, Hainan, Laos, Thailand, Vietnam, and the Western Ghats of India, may acidify to a significant degree on a 0-50 y timescale, depending on individual site management and abiotic and biotic characteristics. To make a clearer assessment of risk, site-specific data are required for soil chemistry and deposition (especially base cation deposition); S and N retention in soils and ecosystems; and biomass harvesting and weathering rates from sites across Asia representative of different soil and vegetation types and management regimes. National and regional assessments of soils using the simple methods described in this paper can provide an appreciation of the time dimension of soil acidification-related impacts and should be useful in planning further studies and, possibly, implementing measures to reduce risks of acidification.

Spatial variation of modelled total, dry and wet nitrogen deposition to forests at global scale.

Forests are an important biome that covers about one third of the global land surface and provides important ecosystem services. Since atmospheric deposition of nitrogen (N) can have both beneficial and deleterious effects, it is important to quantify the amount of N deposition to forest ecosystems. Measurements of N deposition to the numerous forest biomes across the globe are scarce, so chemical transport models are often used to provide estimates of atmospheric N inputs to these ecosystems. We provide an overview of approaches used to calculate N deposition in commonly used chemical transport models. The Task Force on Hemispheric Transport of Air Pollution (HTAP2) study intercompared N deposition values from a number of global chemical transport models. Using a multi-model mean calculated from the HTAP2 deposition values, we map N deposition to global forests to examine spatial variations in total, dry and wet deposition. Highest total N deposition occurs in eastern and southern China, Japan, Eastern U.S. and Europe while the highest dry deposition occurs in tropical forests. The European Monitoring and Evaluation Program (EMEP) model predicts grid-average deposition, but also produces deposition by land use type allowing us to compare deposition specifically to forests with the grid-average value. We found that, for this study, differences between the grid-average and forest specific could be as much as a factor of two and up to more than a factor of five in extreme cases. This suggests that consideration should be given to using forest-specific deposition for input to ecosystem assessments such as critical loads determinations.

HTAP2 multi-model estimates of premature human mortality due to intercontinental transport of air pollution and emission sectors.

Ambient air pollution from ozone and fine particulate matter is associated with premature mortality. As emissions from one continent influence air quality over others, changes in emissions can also influence human health on other continents. We estimate global air pollution-related premature mortality from exposure to PM2.5 and ozone, and the avoided deaths from 20% anthropogenic emission reductions from six source regions, North America (NAM), Europe (EUR), South Asia (SAS), East Asia (EAS), Russia/Belarus/Ukraine (RBU) and the Middle East (MDE), three global emission sectors, Power and Industry (PIN), Ground Transportation (TRN) and Residential (RES) and one global domain (GLO), using an ensemble of global chemical transport model simulations coordinated by the second phase of the Task Force on Hemispheric Transport of Air Pollution (TF-HTAP2), and epidemiologically-derived concentration-response functions. We build on results from previous studies of the TF-HTAP by using improved atmospheric models driven by new estimates of 2010 anthropogenic emissions (excluding methane), with more source and receptor regions, new consideration of source sector impacts, and new epidemiological mortality functions. We estimate 290,000 (95% CI: 30,000, 600,000) premature O3-related deaths and 2.8 million (0.5 million, 4.6 million) PM2.5-related premature deaths globally for the baseline year 2010. While 20% emission reductions from one region generally lead to more avoided deaths within the source region than outside, reducing emissions from MDE and RBU can avoid more O3-related deaths outside of these regions than within, and reducing MDE emissions also avoids more PM2.5-related deaths outside of MDE than within. Our findings that most avoided O3-related deaths from emission reductions in NAM and EUR occur outside of those regions contrast with those of previous studies, while estimates of PM2.5-related deaths from NAM, EUR, SAS and EAS emission reductions agree well. In addition, EUR, MDE and RBU have more avoided O3-related deaths from reducing foreign emissions than from domestic reductions. For six regional emission reductions, the total avoided extra-regional mortality is estimated as 6,000 (-3,400, 15,500) deaths/year and 25,100 (8,200, 35,800) deaths/year through changes in O3 and PM2.5, respectively. Interregional transport of air pollutants leads to more deaths through changes in PM2.5 than in O3, even though O3 is transported more on interregional scales, since PM2.5 has a stronger influence on mortality. For NAM and EUR, our estimates of avoided mortality from regional and extra-regional emission reductions are comparable to those estimated by regional models for these same experiments. In sectoral emission reductions, TRN emissions account for the greatest fraction (26-53% of global emission reduction) of O3-related premature deaths in most regions, in agreement with previous studies, except for EAS (58%) and RBU (38%) where PIN emissions dominate. In contrast, PIN emission reductions have the greatest fraction (38-78% of global emission reduction) of PM2.5-related deaths in most regions, except for SAS (45%) where RES emission dominates, which differs with previous studies in which RES emissions dominate global health impacts. The spread of air pollutant concentration changes across models contributes most to the overall uncertainty in estimated avoided deaths, highlighting the uncertainty in results based on a single model. Despite uncertainties, the health benefits of reduced intercontinental air pollution transport suggest that international cooperation may be desirable to mitigate pollution transported over long distances.

Technical note: Coordination and harmonization of the multi-scale, multi-model activities HTAP2, AQMEII3, and MICS-Asia3: simulations, emission inventories, boundary conditions, and model output formats.

We present an overview of the coordinated global numerical modelling experiments performed during 2012-2016 by the Task Force on Hemispheric Transport of Air Pollution (TF HTAP), the regional experiments by the Air Quality Model Evaluation International Initiative (AQMEII) over Europe and North America, and the Model Intercomparison Study for Asia (MICS-Asia). To improve model estimates of the impacts of intercontinental transport of air pollution on climate, ecosystems, and human health and to answer a set of policy-relevant questions, these three initiatives performed emission perturbation modelling experiments consistent across the global, hemispheric, and continental/regional scales. In all three initiatives, model results are extensively compared against monitoring data for a range of variables (meteorological, trace gas concentrations, and aerosol mass and composition) from different measurement platforms (ground measurements, vertical profiles, airborne measurements) collected from a number of sources. Approximately 10 to 25 modelling groups have contributed to each initiative, and model results have been managed centrally through three data hubs maintained by each initiative. Given the organizational complexity of bringing together these three initiatives to address a common set of policy-relevant questions, this publication provides the motivation for the modelling activity, the rationale for specific choices made in the model experiments, and an overview of the organizational structures for both the modelling and the measurements used and analysed in a number of modelling studies in this special issue.

Observation- and Model-Based Estimates of Particulate Dry Nitrogen Deposition to the Oceans.

Anthropogenic nitrogen (N) emissions to the atmosphere have increased significantly the deposition of nitrate (NO3-) and ammonium (NH4+) to the surface waters of the open ocean, with potential impacts on marine productivity and the global carbon cycle. Global-scale understanding of the impacts of N deposition to the oceans is reliant on our ability to produce and validate models of nitrogen emission, atmospheric chemistry, transport and deposition. In this work, ~2900 observations of aerosol NO3- and NH4+ concentrations, acquired from sampling aboard ships in the period 1995 - 2012, are used to assess the performance of modelled N concentration and deposition fields over the remote ocean. Three ocean regions (the eastern tropical North Atlantic, the northern Indian Ocean and northwest Pacific) were selected, in which the density and distribution of observational data were considered sufficient to provide effective comparison to model products. All of these study regions are affected by transport and deposition of mineral dust, which alters the deposition of N, due to uptake of nitrogen oxides (NOx) on mineral surfaces. Assessment of the impacts of atmospheric N deposition on the ocean requires atmospheric chemical transport models to report deposition fluxes, however these fluxes cannot be measured over the ocean. Modelling studies such as the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP), which only report deposition flux are therefore very difficult to validate for dry deposition. Here the available observational data were averaged over a 5° × 5° grid and compared to ACCMIP dry deposition fluxes (ModDep) of oxidised N (NOy) and reduced N (NHx) and to the following parameters from the TM4-ECPL (TM4) model: ModDep for NOy, NHx and particulate NO3- and NH4+, and surface-level particulate NO3- and NH4+ concentrations. As a model ensemble, ACCMIP can be expected to be more robust than TM4, while TM4 gives access to speciated parameters (NO3- and NH4+) that are more relevant to the observed parameters and which are not available in ACCMIP. Dry deposition fluxes (CalDep) were calculated from the observed concentrations using estimates of dry deposition velocities. Model - observation ratios, weighted by grid-cell area and numbers of observations, (RA,n) were used to assess the performance of the models. Comparison in the three study regions suggests that TM4 over-estimates NO3- concentrations (RA,n = 1.4 - 2.9) and under-estimates NH4+ concentrations (RA,n = 0.5 - 0.7), with spatial distributions in the tropical Atlantic and northern Indian Ocean not being reproduced by the model. In the case of NH4+ in the Indian Ocean, this discrepancy was probably due to seasonal biases in the sampling. Similar patterns were observed in the various comparisons of CalDep to ModDep (RA,n = 0.6 - 2.6 for NO3-, 0.6 - 3.1 for NH4+). Values of RA,n for NHx CalDep - ModDep comparisons were approximately double the corresponding values for NH4+ CalDep - ModDep comparisons due to the significant fraction of gas-phase NH3 deposition incorporated in the TM4 and ACCMIP NHx model products. All of the comparisons suffered due to the scarcity of observational data and the large uncertainty in dry deposition velocities used to derive deposition fluxes from concentrations. These uncertainties have been a major limitation on estimates of the flux of material to the oceans for several decades. Recommendations are made for improvements in N deposition estimation through changes in observations, modelling and model - observation comparison procedures. Validation of modelled dry deposition requires effective comparisons to observable aerosol-phase species concentrations and this cannot be achieved if model products only report dry deposition flux over the ocean.

Impact of intercontinental pollution transport on North American ozone air pollution: an HTAP phase 2 multi-model study.

The recent update on the US National Ambient Air Quality Standards (NAAQS) of the ground-level ozone (O3/ can benefit from a better understanding of its source contributions in different US regions during recent years. In the Hemispheric Transport of Air Pollution experiment phase 1 (HTAP1), various global models were used to determine the O3 source-receptor (SR) relationships among three continents in the Northern Hemisphere in 2001. In support of the HTAP phase 2 (HTAP2) experiment that studies more recent years and involves higher-resolution global models and regional models' participation, we conduct a number of regional-scale Sulfur Transport and dEposition Model (STEM) air quality base and sensitivity simulations over North America during May-June 2010. STEM's top and lateral chemical boundary conditions were downscaled from three global chemical transport models' (i.e., GEOS-Chem, RAQMS, and ECMWF C-IFS) base and sensitivity simulations in which the East Asian (EAS) anthropogenic emissions were reduced by 20 %. The mean differences between STEM surface O3 sensitivities to the emission changes and its corresponding boundary condition model's are smaller than those among its boundary condition models, in terms of the regional/period-mean (<10 %) and the spatial distributions. An additional STEM simulation was performed in which the boundary conditions were downscaled from a RAQMS (Realtime Air Quality Modeling System) simulation without EAS anthropogenic emissions. The scalability of O3 sensitivities to the size of the emission perturbation is spatially varying, and the full (i.e., based on a 100% emission reduction) source contribution obtained from linearly scaling the North American mean O3 sensitivities to a 20% reduction in the EAS anthropogenic emissions may be underestimated by at least 10 %. The three boundary condition models' mean O3 sensitivities to the 20% EAS emission perturbations are ~8% (May-June 2010)/~11% (2010 annual) lower than those estimated by eight global models, and the multi-model ensemble estimates are higher than the HTAP1 reported 2001 conditions. GEOS-Chem sensitivities indicate that the EAS anthropogenic NO x emissions matter more than the other EAS O3 precursors to the North American O3, qualitatively consistent with previous adjoint sensitivity calculations. In addition to the analyses on large spatial-temporal scales relative to the HTAP1, we also show results on subcontinental and event scales that are more relevant to the US air quality management. The EAS pollution impacts are weaker during observed O3 exceedances than on all days in most US regions except over some high-terrain western US rural/remote areas. Satellite O3 (TES, JPL-IASI, and AIRS) and carbon monoxide (TES and AIRS) products, along with surface measurements and model calculations, show that during certain episodes stratospheric O3 intrusions and the transported EAS pollution influenced O3 in the western and the eastern US differently. Free-running (i.e., without chemical data assimilation) global models underpredicted the transported background O3 during these episodes, posing difficulties for STEM to accurately simulate the surface O3 and its source contribution. Although we effectively improved the modeled O3 by incorporating satellite O3 (OMI and MLS) and evaluated the quality of the HTAP2 emission inventory with the Royal Netherlands Meteorological Institute-Ozone Monitoring Instrument (KNMI-OMI) nitrogen dioxide, using observations to evaluate and improve O3 source attribution still remains to be further explored.

Evaluation of the aerosol vertical distribution in global aerosol models through comparison against CALIOP measurements: AeroCom phase II results.

The ability of 11 models in simulating the aerosol vertical distribution from regional to global scales, as part of the second phase of the AeroCom model intercomparison initiative (AeroCom II), is assessed and compared to results of the first phase. The evaluation is performed using a global monthly gridded data set of aerosol extinction profiles built for this purpose from the CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) Layer Product 3.01. Results over 12 subcontinental regions show that five models improved, whereas three degraded in reproducing the interregional variability in Z α0-6 km, the mean extinction height diagnostic, as computed from the CALIOP aerosol profiles over the 0-6 km altitude range for each studied region and season. While the models' performance remains highly variable, the simulation of the timing of the Z α0-6 km peak season has also improved for all but two models from AeroCom Phase I to Phase II. The biases in Z α0-6 km are smaller in all regions except Central Atlantic, East Asia, and North and South Africa. Most of the models now underestimate Z α0-6 km over land, notably in the dust and biomass burning regions in Asia and Africa. At global scale, the AeroCom II models better reproduce the Z α0-6 km latitudinal variability over ocean than over land. Hypotheses for the performance and evolution of the individual models and for the intermodel diversity are discussed. We also provide an analysis of the CALIOP limitations and uncertainties contributing to the differences between the simulations and observations.

The contribution from shipping emissions to air quality and acid deposition in Europe.

A global three-dimensional Lagrangian chemistry-transport model STOCHEM is used to describe the European regional acid deposition and ozone air quality impacts along the Atlantic Ocean seaboard of Europe, from the SO2, NOx, VOCs and CO emissions from international shipping under conditions appropriate to the year 2000. Model-derived total sulfur deposition from international shipping reaches over 200 mg S m(-2) yr(-1) over the southwestern approaches to the British Isles and Brittany. The contribution from international shipping to surface ozone concentrations during the summertime, peaks at about 6 ppb over Ireland, Brittany and Portugal. Shipping emissions act as an external influence on acid deposition and ozone air quality within Europe and may require control actions in the future if strict deposition and air quality targets are to be met.

A boxmodel development to study the relationships between the photo-oxidants and the particles formation in the troposphere.

The model BAGS (Boxmodel for Aerosol and Gasphase Simulations) has been developed. It is composed of two major modules: the first one describes the system of the chemical reactions in the gaseous phase, the second one calculates the aerosol chemical composition and the dimensional distribution of the particles. The boxmodel has been developed with the introduction of new chemical and physical processes, not previously included, in particular the formation of Secondary Organic Aerosol. The other implemented processes are a module for the dynamic of the particle population, nucleation, coagulation and dry deposition. The last phase of the work has been a check of the BAGS capabilities by a series of tests, that have permitted to compare it with other models (MAPS and MADM). The tests in particular have concerned the aerosol water content prediction, the photochemistry, the condensation of the inorganic compounds and the formation of Secondary Organic Aerosol.

Trend analysis from 1970 to 2008 and model evaluation of EDGARv4 global gridded anthropogenic mercury emissions.

The Emission Database for Global Atmospheric Research (EDGAR) provides a time-series of man-made emissions of greenhouse gases and short-lived atmospheric pollutants from 1970 to 2008. Mercury is included in EDGARv4.tox1, thereby enriching the spectrum of multi-pollutant sources in the database. With an average annual growth rate of 1.3% since 1970, EDGARv4 estimates that the global mercury emissions reached 1,287 tonnes in 2008. Specifically, gaseous elemental mercury (GEM) (Hg(0)) accounted for 72% of the global total emissions, while gaseous oxidised mercury (GOM) (Hg(2+)) and particle bound mercury (PBM) (Hg-P) accounted for only 22% and 6%, respectively. The less reactive form, i.e., Hg(0), has a long atmospheric residence time and can be transported long distances from the emission sources. The artisanal and small-scale gold production, accounted for approximately half of the global Hg(0) emissions in 2008 followed by combustion (29%), cement production (12%) and other metal industry (10%). Given the local-scale impacts of mercury, special attention was given to the spatial distribution showing the emission hot-spots on gridded 0.1°×0.1° resolution maps using detailed proxy data. The comprehensive ex-post analysis of the mitigation of mercury emissions by end-of-pipe abatement measures in the power generation sector and technology changes in the chlor-alkali industry over four decades indicates reductions of 46% and 93%, respectively. Combined, the improved technologies and mitigation measures in these sectors accounted for 401.7 tonnes of avoided mercury emissions in 2008. A comparison shows that EDGARv4 anthropogenic emissions are nearly equivalent to the lower estimates of the United Nations Environment Programme (UNEP)'s mercury emissions inventory for 2005 for most sectors. An evaluation of the EDGARv4 global mercury emission inventory, including mercury speciation, was performed using the GEOS-Chem global 3-D mercury model. The model can generally reproduce both spatial variations and long-term trends in total gaseous mercury concentrations and wet deposition fluxes.